Biological Applications of Hybrid Quantum Mechanics/Molecular Mechanics Calculation
Directory of Open Access Journals (Sweden)
Jiyoung Kang
2012-01-01
Full Text Available Since in most cases biological macromolecular systems including solvent water molecules are remarkably large, the computational costs of performing ab initio calculations for the entire structures are prohibitive. Accordingly, QM calculations that are jointed with MM calculations are crucial to evaluate the long-range electrostatic interactions, which significantly affect the electronic structures of biological macromolecules. A UNIX-shell-based interface program connecting the quantum mechanics (QMs and molecular mechanics (MMs calculation engines, GAMESS and AMBER, was developed in our lab. The system was applied to a metalloenzyme, azurin, and PU.1-DNA complex; thereby, the significance of the environmental effects on the electronic structures of the site of interest was elucidated. Subsequently, hybrid QM/MM molecular dynamics (MD simulation using the calculation system was employed for investigation of mechanisms of hydrolysis (editing reaction in leucyl-tRNA synthetase complexed with the misaminoacylated tRNALeu, and a novel mechanism of the enzymatic reaction was revealed. Thus, our interface program can play a critical role as a powerful tool for state-of-the-art sophisticated hybrid ab initio QM/MM MD simulations of large systems, such as biological macromolecules.
Bryce, Richard A; Hillier, Ian H
2014-01-01
The use of computational quantum chemical methods to aid drug discovery is surveyed. An overview of the various computational models spanning ab initio, density function theory, semiempirical molecular orbital (MO), and hybrid quantum mechanical (QM)/molecular mechanical (MM) methods is given and their strengths and weaknesses are highlighted, focussing on the challenge of obtaining the accuracy essential for them to make a meaningful contribution to drug discovery. Particular attention is given to hybrid QM/MM and semiempirical MO methods which have the potential to yield the necessary accurate predictions of macromolecular structure and reactivity. These methods are shown to have advanced the study of many aspects of substrate-ligand interactions relevant to drug discovery. Thus, the successful parametrization of semiempirical MO methods and QM/MM methods can be used to model noncovalent substrate-protein interactions, and to lead to improved scoring functions. QM/MM methods can be used in crystal structure refinement and are particularly valuable for modelling covalent protein-ligand interactions and can thus aid the design of transition state analogues. An extensive collection of examples from the areas of metalloenzyme structure, enzyme inhibition, and ligand binding affinities and scoring functions are used to illustrate the power of these techniques.
Bayse, Craig A; Merz, Kenneth M
2014-08-05
Understanding the mechanism of prenyltransferases is important to the design of engineered proteins capable of synthesizing derivatives of naturally occurring therapeutic agents. CloQ is a Mg(2+)-independent aromatic prenyltransferase (APTase) that transfers a dimethylallyl group to 4-hydroxyphenylpyruvate in the biosynthetic pathway for clorobiocin. APTases consist of a common ABBA fold that defines a β-barrel containing the reaction cavity. Positively charged basic residues line the inside of the β-barrel of CloQ to activate the pyrophosphate leaving group to replace the function of the Mg(2+) cofactor in other APTases. Classical molecular dynamics simulations of CloQ, its E281G and F68S mutants, and the related NovQ were used to explore the binding of the 4-hydroxyphenylpyruvate (4HPP) and dimethylallyl diphosphate substrates in the reactive cavity and the role of various conserved residues. Hybrid quantum mechanics/molecular mechanics potential of mean force (PMF) calculations show that the effect of the replacement of the Mg(2+) cofactor with basic residues yields a similar activation barrier for prenylation to Mg(2+)-dependent APTases like NphB. The topology of the binding pocket for 4HPP is important for selective prenylation at the ortho position of the ring. Methylation at this position alters the conformation of the substrate for O-prenylation at the phenol group. Further, a two-dimensional PMF scan shows that a "reverse" prenylation product may be a possible target for protein engineering.
Huang, Jing; Mei, Ye; König, Gerhard; Simmonett, Andrew C; Pickard, Frank C; Wu, Qin; Wang, Lee-Ping; MacKerell, Alexander D; Brooks, Bernard R; Shao, Yihan
2017-02-14
In this work, we report two polarizable molecular mechanics (polMM) force field models for estimating the polarization energy in hybrid quantum mechanical molecular mechanical (QM/MM) calculations. These two models, named the potential of atomic charges (PAC) and potential of atomic dipoles (PAD), are formulated from the ab initio quantum mechanical (QM) response kernels for the prediction of the QM density response to an external molecular mechanical (MM) environment (as described by external point charges). The PAC model is similar to fluctuating charge (FQ) models because the energy depends on external electrostatic potential values at QM atomic sites; the PAD energy depends on external electrostatic field values at QM atomic sites, resembling induced dipole (ID) models. To demonstrate their uses, we apply the PAC and PAD models to 12 small molecules, which are solvated by TIP3P water. The PAC model reproduces the QM/MM polarization energy with a R 2 value of 0.71 for aniline (in 10,000 TIP3P water configurations) and 0.87 or higher for other 11 solute molecules, while the PAD model has a much better performance with R 2 values of 0.98 or higher. The PAC model reproduces reference QM/MM hydration free energies for 12 solute molecules with a RMSD of 0.59 kcal/mol. The PAD model is even more accurate, with a much smaller RMSD of 0.12 kcal/mol, with respect to the reference. This suggests that polarization effects, including both local charge distortion and intramolecular charge transfer, can be well captured by induced dipole type models with proper parametrization.
Sokkar, Pandian; Boulanger, Eliot; Thiel, Walter; Sanchez-Garcia, Elsa
2015-04-14
We present a hybrid quantum mechanics/molecular mechanics/coarse-grained (QM/MM/CG) multiresolution approach for solvated biomolecular systems. The chemically important active-site region is treated at the QM level. The biomolecular environment is described by an atomistic MM force field, and the solvent is modeled with the CG Martini force field using standard or polarizable (pol-CG) water. Interactions within the QM, MM, and CG regions, and between the QM and MM regions, are treated in the usual manner, whereas the CG-MM and CG-QM interactions are evaluated using the virtual sites approach. The accuracy and efficiency of our implementation is tested for two enzymes, chorismate mutase (CM) and p-hydroxybenzoate hydroxylase (PHBH). In CM, the QM/MM/CG potential energy scans along the reaction coordinate yield reaction energies that are too large, both for the standard and polarizable Martini CG water models, which can be attributed to adverse effects of using large CG water beads. The inclusion of an atomistic MM water layer (10 Å for uncharged CG water and 5 Å for polarizable CG water) around the QM region improves the energy profiles compared to the reference QM/MM calculations. In analogous QM/MM/CG calculations on PHBH, the use of the pol-CG description for the outer water does not affect the stabilization of the highly charged FADHOOH-pOHB transition state compared to the fully atomistic QM/MM calculations. Detailed performance analysis in a glycine-water model system indicates that computation times for QM energy and gradient evaluations at the density functional level are typically reduced by 40-70% for QM/MM/CG relative to fully atomistic QM/MM calculations.
Faheem, Muhammad; Heyden, Andreas
2014-08-12
We report the development of a quantum mechanics/molecular mechanics free energy perturbation (QM/MM-FEP) method for modeling chemical reactions at metal-water interfaces. This novel solvation scheme combines planewave density function theory (DFT), periodic electrostatic embedded cluster method (PEECM) calculations using Gaussian-type orbitals, and classical molecular dynamics (MD) simulations to obtain a free energy description of a complex metal-water system. We derive a potential of mean force (PMF) of the reaction system within the QM/MM framework. A fixed-size, finite ensemble of MM conformations is used to permit precise evaluation of the PMF of QM coordinates and its gradient defined within this ensemble. Local conformations of adsorbed reaction moieties are optimized using sequential MD-sampling and QM-optimization steps. An approximate reaction coordinate is constructed using a number of interpolated states and the free energy difference between adjacent states is calculated using the QM/MM-FEP method. By avoiding on-the-fly QM calculations and by circumventing the challenges associated with statistical averaging during MD sampling, a computational speedup of multiple orders of magnitude is realized. The method is systematically validated against the results of ab initio QM calculations and demonstrated for C-C cleavage in double-dehydrogenated ethylene glycol on a Pt (111) model surface.
Asadi, Parvin; Khodarahmi, Ghadamali; Farrokhpour, Hossein; Hassanzadeh, Farshid; Saghaei, Lotfollah
2017-06-01
In an attempt to identify some new potential leads as anti-breast cancer agents, novel hybrid compounds were designed by molecular hybridization approach. These derivatives were structurally derived from hybrid benzofuran-imidazole and quinazolinone derivatives, which had shown good cytotoxicity against the breast cancer cell line (MCF-7). Since aromatase enzyme (CYP19) is highly expressed in the MCF-7 cell line, the binding of these novel hybrid compounds to aromatase was investigated using the docking method. In this study, due to the positive charge on the imidazole ring of the designed ligands and also, the presence of heme iron in the active site of the enzyme, it was decided to optimize the ligand inside the protein to obtain more realistic atomic charges for it. Quantum mechanical/molecular mechanical (QM/MM) method was used to obtain more accurate atomic charges of ligand for docking calculations by considering the polarization effects of CYP19 on ligands. It was observed that the refitted charge improved the binding energy of the docked compounds. Also, the results showed that these novel hybrid compounds were adopted properly within the aromatase binding site, thereby suggesting that they could be potential inhibitors of aromatase. The main binding modes in these complexes were through hydrophobic and H bond interactions showing agreement with the basic physicochemical features of known anti aromatase compounds. Finally, the complex structures obtained from the docking study were used for single point QM/MM calculations to obtain more accurate electronic interaction energy, considering the electronic polarization of the ligand by its protein environment.
Kraus, Jodi; Gupta, Rupal; Yehl, Jenna; Lu, Manman; Case, David A; Gronenborn, Angela M; Akke, Mikael; Polenova, Tatyana
2018-03-22
Magic angle spinning NMR spectroscopy is uniquely suited to probe the structure and dynamics of insoluble proteins and protein assemblies at atomic resolution, with NMR chemical shifts containing rich information about biomolecular structure. Access to this information, however, is problematic, since accurate quantum mechanical calculation of chemical shifts in proteins remains challenging, particularly for 15 N H . Here we report on isotropic chemical shift predictions for the carbohydrate recognition domain of microcrystalline galectin-3, obtained from using hybrid quantum mechanics/molecular mechanics (QM/MM) calculations, implemented using an automated fragmentation approach, and using very high resolution (0.86 Å lactose-bound and 1.25 Å apo form) X-ray crystal structures. The resolution of the X-ray crystal structure used as an input into the AF-NMR program did not affect the accuracy of the chemical shift calculations to any significant extent. Excellent agreement between experimental and computed shifts is obtained for 13 C α , while larger scatter is observed for 15 N H chemical shifts, which are influenced to a greater extent by electrostatic interactions, hydrogen bonding, and solvation.
Bryce, Richard A.; Vincent, Mark A.; Malcolm, Nathaniel O. J.; Hillier, Ian H.; Burton, Neil A.
1998-08-01
A new hybrid quantum mechanical/molecular mechanical model of solvation is developed and used to describe the structure and dynamics of small fluoride/water clusters, using an ab initio wave function to model the ion and a fluctuating charge potential to model the waters. Appropriate parameters for the water-water and fluoride-water interactions are derived, with the fluoride anion being described by density functional theory and a large Gaussian basis. The role of solvent polarization in determining the structure and energetics of F(H2O)4- clusters is investigated, predicting a slightly greater stability of the interior compared to the surface structure, in agreement with ab initio studies. An extended Lagrangian treatment of the polarizable water, in which the water atomic charges fluctuate dynamically, is used to study the dynamics of F(H2O)4- cluster. A simulation using a fixed solvent charge distribution indicates principally interior, solvated states for the cluster. However, a preponderance of trisolvated configurations is observed using the polarizable model at 300 K, which involves only three direct fluoride-water hydrogen bonds. Ab initio calculations confirm this trisolvated species as a thermally accessible state at room temperature, in addition to the tetrasolvated interior and surface structures. Extension of this polarizable water model to fluoride clusters with five and six waters gave less satisfactory agreement with experimental energies and with ab initio geometries. However, our results do suggest that a quantitative model of solvent polarization is fundamental for an accurate understanding of the properties of anionic water clusters.
Quantum Mechanics/Molecular Mechanics Modeling of Drug Metabolism
DEFF Research Database (Denmark)
Lonsdale, Richard; Fort, Rachel M; Rydberg, Patrik
2016-01-01
)-mexiletine in CYP1A2 with hybrid quantum mechanics/molecular mechanics (QM/MM) methods, providing a more detailed and realistic model. Multiple reaction barriers have been calculated at the QM(B3LYP-D)/MM(CHARMM27) level for the direct N-oxidation and H-abstraction/rebound mechanisms. Our calculated barriers......The mechanism of cytochrome P450(CYP)-catalyzed hydroxylation of primary amines is currently unclear and is relevant to drug metabolism; previous small model calculations have suggested two possible mechanisms: direct N-oxidation and H-abstraction/rebound. We have modeled the N-hydroxylation of (R...... indicate that the direct N-oxidation mechanism is preferred and proceeds via the doublet spin state of Compound I. Molecular dynamics simulations indicate that the presence of an ordered water molecule in the active site assists in the binding of mexiletine in the active site...
Exact and Optimal Quantum Mechanics/Molecular Mechanics Boundaries.
Sun, Qiming; Chan, Garnet Kin-Lic
2014-09-09
Motivated by recent work in density matrix embedding theory, we define exact link orbitals that capture all quantum mechanical (QM) effects across arbitrary quantum mechanics/molecular mechanics (QM/MM) boundaries. Exact link orbitals are rigorously defined from the full QM solution, and their number is equal to the number of orbitals in the primary QM region. Truncating the exact set yields a smaller set of link orbitals optimal with respect to reproducing the primary region density matrix. We use the optimal link orbitals to obtain insight into the limits of QM/MM boundary treatments. We further analyze the popular general hybrid orbital (GHO) QM/MM boundary across a test suite of molecules. We find that GHOs are often good proxies for the most important optimal link orbital, although there is little detailed correlation between the detailed GHO composition and optimal link orbital valence weights. The optimal theory shows that anions and cations cannot be described by a single link orbital. However, expanding to include the second most important optimal link orbital in the boundary recovers an accurate description. The second optimal link orbital takes the chemically intuitive form of a donor or acceptor orbital for charge redistribution, suggesting that optimal link orbitals can be used as interpretative tools for electron transfer. We further find that two optimal link orbitals are also sufficient for boundaries that cut across double bonds. Finally, we suggest how to construct "approximately" optimal link orbitals for practical QM/MM calculations.
Shen, Lin; Yang, Weitao
2016-04-12
We developed a new multiresolution method that spans three levels of resolution with quantum mechanical, atomistic molecular mechanical, and coarse-grained models. The resolution-adapted all-atom and coarse-grained water model, in which an all-atom structural description of the entire system is maintained during the simulations, is combined with the ab initio quantum mechanics and molecular mechanics method. We apply this model to calculate the redox potentials of the aqueous ruthenium and iron complexes by using the fractional number of electrons approach and thermodynamic integration simulations. The redox potentials are recovered in excellent accordance with the experimental data. The speed-up of the hybrid all-atom and coarse-grained water model renders it computationally more attractive. The accuracy depends on the hybrid all-atom and coarse-grained water model used in the combined quantum mechanical and molecular mechanical method. We have used another multiresolution model, in which an atomic-level layer of water molecules around redox center is solvated in supramolecular coarse-grained waters for the redox potential calculations. Compared with the experimental data, this alternative multilayer model leads to less accurate results when used with the coarse-grained polarizable MARTINI water or big multipole water model for the coarse-grained layer.
Simulation with quantum mechanics/molecular mechanics for drug discovery.
Barbault, Florent; Maurel, François
2015-10-01
Biological macromolecules, such as proteins or nucleic acids, are (still) molecules and thus they follow the same chemical rules that any simple molecule follows, even if their size generally renders accurate studies unhelpful. However, in the context of drug discovery, a detailed analysis of ligand association is required for understanding or predicting their interactions and hybrid quantum mechanics/molecular mechanics (QM/MM) computations are relevant tools to help elucidate this process. In this review, the authors explore the use of QM/MM for drug discovery. After a brief description of the molecular mechanics (MM) technique, the authors describe the subtractive and additive techniques for QM/MM computations. The authors then present several application cases in topics involved in drug discovery. QM/MM have been widely employed during the last decades to study chemical processes such as enzyme-inhibitor interactions. However, despite the enthusiasm around this area, plain MM simulations may be more meaningful than QM/MM. To obtain reliable results, the authors suggest fixing several keystone parameters according to the underlying chemistry of each studied system.
Hu, Hao; Liu, Haiyan
2013-05-30
Developments in computing hardware and algorithms have made direct molecular dynamics simulation with the combined quantum mechanical/molecular mechanical methods affordable for small solute molecules in solution, in which much improved accuracy can be obtained via the quantum mechanical treatment of the solute molecule and even sometimes water molecules in the first solvation shell. However, unlike the conventional molecular mechanical simulations of large molecules, e.g., proteins, in solutions, special care must be taken in the technical details of the simulation, including the thermostat of the solute/solvent system, so that the conformational space of the solute molecules can be properly sampled. We show here that the common setup for classical molecular mechanical molecular dynamics simulations, such as the Berendsen or single Nose-Hoover thermostat, and/or rigid water models could lead to pathological sampling of the solutes' conformation. In the extreme example of a methanol molecule in aqueous solution, improper and sluggish setups could generate two peaks in the distribution of the O-H bond length. We discuss the factors responsible for this somewhat unexpected result and evoke a simple and ancient technical fix-up to resolve this problem.
International Nuclear Information System (INIS)
Lamare, V.; Golebiowski, J.; Ruiz-Lopez, M.F.; Martins-Costa, M.; Millot, C.
2000-01-01
Calixarene-crown-6s in 1,3-alternate conformation are compounds currently investigated for their ability to selectively extract traces of cesium from acidic or strong salinity aqueous solutions. Studies based on molecular modeling were undertaken on these systems to understand their behavior regarding cesium and other alkali cations, in particular sodium. In this work, a recently developed molecular modeling approach was used to investigate calixarene BC6 and its alkali complexes. The whole calixarene ligand is treated by the semiempirical AM1 quantum method (QM) whereas the cation and solvent are treated by a conventional force field (MM). The total energy of the system is the sum of the QM and MM sub-system contributions plus the QM/MM interaction energy. The latter includes the electrostatic interaction between QM charges (nuclei + electrons) and MM sites, and the non-electrostatic QM/MM van der Weals term, usually expressed by a Lennard-Jones potential. In the QM/MM method, van der Waals interactions between the QM and MM sub-systems are described by empirical Lennard-Jones parameters which must be adapted to the hybrid potential considered. Parameters on oxygen atoms were optimized. For the cations, two sets of Parameters were tested: Aqvist empirical parameters, derived to represent cation/water interactions in classical dynamics (set 2), and a new set of parameters which we calculated from dispersion coefficients available in the literature (set 1). The latter gave better results for the interactions with the crown. In the sodium complex, the cation interacts with only four oxygen atoms of the crown, whereas in the complex with cesium, the interaction involves six oxygen atoms. Distortion of the BC6 is therefore less with sodium and favors the corresponding complex by 4 kcal/mol. The cation/BC6 van der Waals energy is very weak for the two complexes. Hence the interaction between the cation and BC6 is primarily electrostatic. The BC6 polarization energy due
Quantum Mechanics/Molecular Mechanics Study of the Sialyltransferase Reaction Mechanism.
Hamada, Yojiro; Kanematsu, Yusuke; Tachikawa, Masanori
2016-10-11
The sialyltransferase is an enzyme that transfers the sialic acid moiety from cytidine 5'-monophospho-N-acetyl-neuraminic acid (CMP-NeuAc) to the terminal position of glycans. To elucidate the catalytic mechanism of sialyltransferase, we explored the potential energy surface along the sialic acid transfer reaction coordinates by the hybrid quantum mechanics/molecular mechanics method on the basis of the crystal structure of sialyltransferase CstII. Our calculation demonstrated that CstII employed an S N 1-like reaction mechanism via the formation of a short-lived oxocarbenium ion intermediate. The computational barrier height was 19.5 kcal/mol, which reasonably corresponded with the experimental reaction rate. We also found that two tyrosine residues (Tyr156 and Tyr162) played a vital role in stabilizing the intermediate and the transition states by quantum mechanical interaction with CMP.
Multiscale Quantum Mechanics/Molecular Mechanics Simulations with Neural Networks.
Shen, Lin; Wu, Jingheng; Yang, Weitao
2016-10-11
Molecular dynamics simulation with multiscale quantum mechanics/molecular mechanics (QM/MM) methods is a very powerful tool for understanding the mechanism of chemical and biological processes in solution or enzymes. However, its computational cost can be too high for many biochemical systems because of the large number of ab initio QM calculations. Semiempirical QM/MM simulations have much higher efficiency. Its accuracy can be improved with a correction to reach the ab initio QM/MM level. The computational cost on the ab initio calculation for the correction determines the efficiency. In this paper we developed a neural network method for QM/MM calculation as an extension of the neural-network representation reported by Behler and Parrinello. With this approach, the potential energy of any configuration along the reaction path for a given QM/MM system can be predicted at the ab initio QM/MM level based on the semiempirical QM/MM simulations. We further applied this method to three reactions in water to calculate the free energy changes. The free-energy profile obtained from the semiempirical QM/MM simulation is corrected to the ab initio QM/MM level with the potential energies predicted with the constructed neural network. The results are in excellent accordance with the reference data that are obtained from the ab initio QM/MM molecular dynamics simulation or corrected with direct ab initio QM/MM potential energies. Compared with the correction using direct ab initio QM/MM potential energies, our method shows a speed-up of 1 or 2 orders of magnitude. It demonstrates that the neural network method combined with the semiempirical QM/MM calculation can be an efficient and reliable strategy for chemical reaction simulations.
Ibrahim, Mahmoud A A
2011-10-24
The performance of semiempirical molecular-orbital methods--MNDO, MNDO-d, AM1, RM1, PM3 and PM6--in describing halogen bonding was evaluated, and the results were compared with molecular mechanical (MM) and quantum mechanical (QM) data. Three types of performance were assessed: (1) geometrical optimizations and binding energy calculations for 27 halogen-containing molecules complexed with various Lewis bases (Two of the tested methods, AM1 and RM1, gave results that agree with the QM data.); (2) charge distribution calculations for halobenzene molecules, determined by calculating the solvation free energies of the molecules relative to benzene in explicit and implicit generalized Born (GB) solvents (None of the methods gave results that agree with the experimental data.); and (3) appropriateness of the semiempirical methods in the hybrid quantum-mechanical/molecular-mechanical (QM/MM) scheme, investigated by studying the molecular inhibition of CK2 protein by eight halobenzimidazole and -benzotriazole derivatives using hybrid QM/MM molecular-dynamics (MD) simulations with the inhibitor described at the QM level by the AM1 method and the rest of the system described at the MM level. The pure MM approach with inclusion of an extra point of positive charge on the halogen atom approach gave better results than the hybrid QM/MM approach involving the AM1 method. Also, in comparison with the pure MM-GBSA (generalized Born surface area) binding energies and experimental data, the calculated QM/MM-GBSA binding energies of the inhibitors were improved by replacing the G(GB,QM/MM) solvation term with the corresponding G(GB,MM) term.
Hybrid quantum information processing
Energy Technology Data Exchange (ETDEWEB)
Furusawa, Akira [Department of Applied Physics, School of Engineering, The University of Tokyo (Japan)
2014-12-04
I will briefly explain the definition and advantage of hybrid quantum information processing, which is hybridization of qubit and continuous-variable technologies. The final goal would be realization of universal gate sets both for qubit and continuous-variable quantum information processing with the hybrid technologies. For that purpose, qubit teleportation with a continuousvariable teleporter is one of the most important ingredients.
A quantum-mechanics molecular-mechanics scheme for extended systems.
Hunt, Diego; Sanchez, Veronica M; Scherlis, Damián A
2016-08-24
We introduce and discuss a hybrid quantum-mechanics molecular-mechanics (QM-MM) approach for Car-Parrinello DFT simulations with pseudopotentials and planewaves basis, designed for the treatment of periodic systems. In this implementation the MM atoms are considered as additional QM ions having fractional charges of either sign, which provides conceptual and computational simplicity by exploiting the machinery already existing in planewave codes to deal with electrostatics in periodic boundary conditions. With this strategy, both the QM and MM regions are contained in the same supercell, which determines the periodicity for the whole system. Thus, while this method is not meant to compete with non-periodic QM-MM schemes able to handle extremely large but finite MM regions, it is shown that for periodic systems of a few hundred atoms, our approach provides substantial savings in computational times by treating classically a fraction of the particles. The performance and accuracy of the method is assessed through the study of energetic, structural, and dynamical aspects of the water dimer and of the aqueous bulk phase. Finally, the QM-MM scheme is applied to the computation of the vibrational spectra of water layers adsorbed at the TiO2 anatase (1 0 1) solid-liquid interface. This investigation suggests that the inclusion of a second monolayer of H2O molecules is sufficient to induce on the first adsorbed layer, a vibrational dynamics similar to that taking place in the presence of an aqueous environment. The present QM-MM scheme appears as a very interesting tool to efficiently perform molecular dynamics simulations of complex condensed matter systems, from solutions to nanoconfined fluids to different kind of interfaces.
A quantum-mechanics molecular-mechanics scheme for extended systems
International Nuclear Information System (INIS)
Hunt, Diego; Scherlis, Damián A; Sanchez, Veronica M
2016-01-01
We introduce and discuss a hybrid quantum-mechanics molecular-mechanics (QM-MM) approach for Car–Parrinello DFT simulations with pseudopotentials and planewaves basis, designed for the treatment of periodic systems. In this implementation the MM atoms are considered as additional QM ions having fractional charges of either sign, which provides conceptual and computational simplicity by exploiting the machinery already existing in planewave codes to deal with electrostatics in periodic boundary conditions. With this strategy, both the QM and MM regions are contained in the same supercell, which determines the periodicity for the whole system. Thus, while this method is not meant to compete with non-periodic QM-MM schemes able to handle extremely large but finite MM regions, it is shown that for periodic systems of a few hundred atoms, our approach provides substantial savings in computational times by treating classically a fraction of the particles. The performance and accuracy of the method is assessed through the study of energetic, structural, and dynamical aspects of the water dimer and of the aqueous bulk phase. Finally, the QM-MM scheme is applied to the computation of the vibrational spectra of water layers adsorbed at the TiO 2 anatase (1 0 1) solid–liquid interface. This investigation suggests that the inclusion of a second monolayer of H 2 O molecules is sufficient to induce on the first adsorbed layer, a vibrational dynamics similar to that taking place in the presence of an aqueous environment. The present QM-MM scheme appears as a very interesting tool to efficiently perform molecular dynamics simulations of complex condensed matter systems, from solutions to nanoconfined fluids to different kind of interfaces. (paper)
Canaval, Lorenz R; Lutz, Oliver M D; Weiss, Alexander K H; Huck, Christian W; Hofer, Thomas S
2014-11-17
This work presents a hybrid ab initio quantum mechanical/molecular mechanical simulation at the RI-MP2 level of theory investigating the hydrolysis process of arsenic(III), ultimately leading to arsenous acid (H3AsO3). A newly implemented dissociative water model has been applied to treat the interactions in the classical region, which is capable of describing non-neutral water species such as hydroxide and oxonium ions. Three stages of hydrolysis have been observed during the simulation and besides profound dynamical considerations, detailed insights into structural changes and atomic partial charge shifts are presented. In particular, the geometrical properties of H-bonds involved in each of the three proton transfer events and subsequent proton hopping reactions are discussed. A Laguerre tessellation analysis has been employed to estimate the molecular volume of H3AsO3. Estimations of pKa values of the arsenic(III)-aquo-complexes have been obtained at the G4 and CBS-Q//B3 levels of theory using a thermodynamic cycle, whereas rate constants for the final hydrolysis step have been determined via reaction path optimization and transition state theory. Newly recorded Fourier transform infrared (FT-IR) spectroscopy measurements have been compared to power spectra obtained from the simulation data, confirming its quality. The simulation findings, as well as results from computational spectroscopic calculations utilizing the PT2-VSCF methodology, proved valuable for the interpretation of the experimental FT-IR data, elucidating the particularities of the strongly observed IR Raman noncoincidence effect.
Świderek, Katarzyna; Arafet, Kemel; Kohen, Amnon; Moliner, Vicent
2017-03-14
Given the ubiquity of hydride-transfer reactions in enzyme-catalyzed processes, identifying the appropriate computational method for evaluating such biological reactions is crucial to perform theoretical studies of these processes. In this paper, the hydride-transfer step catalyzed by thymidylate synthase (TSase) is studied by examining hybrid quantum mechanics/molecular mechanics (QM/MM) potentials via multiple semiempirical methods and the M06-2X hybrid density functional. Calculations of protium and tritium transfer in these reactions across a range of temperatures allowed calculation of the temperature dependence of kinetic isotope effects (KIE). Dynamics and quantum-tunneling effects are revealed to have little effect on the reaction rate, but are significant in determining the KIEs and their temperature dependence. A good agreement with experiments is found, especially when computed for RM1/MM simulations. The small temperature dependence of quantum tunneling corrections and the quasiclassical contribution term cancel each other, while the recrossing transmission coefficient seems to be temperature-independent over the interval of 5-40 °C.
Mendieta-Moreno, Jesús I; Trabada, Daniel G; Mendieta, Jesús; Lewis, James P; Gómez-Puertas, Paulino; Ortega, José
2016-11-03
The absorption of ultraviolet radiation by DNA may result in harmful genetic lesions that affect DNA replication and transcription, ultimately causing mutations, cancer, and/or cell death. We analyze the most abundant photochemical reaction in DNA, the cyclobutane thymine dimer, using hybrid quantum mechanics/molecular mechanics (QM/MM) techniques and QM/MM nonadiabatic molecular dynamics. We find that, due to its double helix structure, DNA presents a free energy barrier between nonreactive and reactive conformations leading to the photolesion. Moreover, our nonadiabatic simulations show that most of the photoexcited reactive conformations return to standard B-DNA conformations after an ultrafast nonradiative decay to the ground state. This work highlights the importance of dynamical effects (free energy, excited-state dynamics) for the study of photochemical reactions in biological systems.
Parks, Jerry M; Hu, Hao; Cohen, Aron J; Yang, Weitao
2008-10-21
The pseudobond method is used in quantum mechanical/molecular mechanical (QM/MM) simulations in which a covalent bond connects the quantum mechanical and classical subsystems. In this method, the molecular mechanical boundary atom is replaced by a special quantum mechanical atom with one free valence that forms a bond with the rest of the quantum mechanical subsystem. This boundary atom is modified through the use of a parametrized effective core potential and basis set. The pseudobond is designed to reproduce the properties of the covalent bond that it has replaced, while invoking as small a perturbation as possible on the system. Following the work of Zhang [J. Chem. Phys. 122, 024114 (2005)], we have developed new pseudobond parameters for use in the simulation of enzymatic systems. Our parameters yield improved electrostatics and deprotonation energies, while at the same time maintaining accurate geometries. We provide parameters for C(ps)(sp(3))-C(sp(3)), C(ps)(sp(3))-C(sp(2),carbonyl), and C(ps)(sp(3))-N(sp(3)) pseudobonds, which allow the interface between the quantum mechanical and molecular mechanical subsystems to be constructed at either the C(alpha)-C(beta) bond of a given amino acid residue or along the peptide backbone. In addition, we demonstrate the efficiency of our parametrization method by generating residue-specific pseudobond parameters for a single amino acid. Such an approach may enable higher accuracy than general purpose parameters for specific QM/MM applications.
Wu, Jingheng; Shen, Lin; Yang, Weitao
2017-10-28
Ab initio quantum mechanics/molecular mechanics (QM/MM) molecular dynamics simulation is a useful tool to calculate thermodynamic properties such as potential of mean force for chemical reactions but intensely time consuming. In this paper, we developed a new method using the internal force correction for low-level semiempirical QM/MM molecular dynamics samplings with a predefined reaction coordinate. As a correction term, the internal force was predicted with a machine learning scheme, which provides a sophisticated force field, and added to the atomic forces on the reaction coordinate related atoms at each integration step. We applied this method to two reactions in aqueous solution and reproduced potentials of mean force at the ab initio QM/MM level. The saving in computational cost is about 2 orders of magnitude. The present work reveals great potentials for machine learning in QM/MM simulations to study complex chemical processes.
Feldt, Jonas; Miranda, Sebastião; Pratas, Frederico; Roma, Nuno; Tomás, Pedro; Mata, Ricardo A
2017-12-28
In this work, we present an optimized perturbative quantum mechanics/molecular mechanics (QM/MM) method for use in Metropolis Monte Carlo simulations. The model adopted is particularly tailored for the simulation of molecular systems in solution but can be readily extended to other applications, such as catalysis in enzymatic environments. The electrostatic coupling between the QM and MM systems is simplified by applying perturbation theory to estimate the energy changes caused by a movement in the MM system. This approximation, together with the effective use of GPU acceleration, leads to a negligible added computational cost for the sampling of the environment. Benchmark calculations are carried out to evaluate the impact of the approximations applied and the overall computational performance.
Rosnik, Andreana M; Curutchet, Carles
2015-12-08
Over the past decade, both experimentalists and theorists have worked to develop methods to describe pigment-protein coupling in photosynthetic light-harvesting complexes in order to understand the molecular basis of quantum coherence effects observed in photosynthesis. Here we present an improved strategy based on the combination of quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulations and excited-state calculations to predict the spectral density of electronic-vibrational coupling. We study the water-soluble chlorophyll-binding protein (WSCP) reconstituted with Chl a or Chl b pigments as the system of interest and compare our work with data obtained by Pieper and co-workers from differential fluorescence line-narrowing spectra (Pieper et al. J. Phys. Chem. B 2011, 115 (14), 4042-4052). Our results demonstrate that the use of QM/MM MD simulations where the nuclear positions are still propagated at the classical level leads to a striking improvement of the predicted spectral densities in the middle- and high-frequency regions, where they nearly reach quantitative accuracy. This demonstrates that the so-called "geometry mismatch" problem related to the use of low-quality structures in QM calculations, not the quantum features of pigments high-frequency motions, causes the failure of previous studies relying on similar protocols. Thus, this work paves the way toward quantitative predictions of pigment-protein coupling and the comprehension of quantum coherence effects in photosynthesis.
Computing pKa Values with a Mixing Hamiltonian Quantum Mechanical/Molecular Mechanical Approach.
Liu, Yang; Fan, Xiaoli; Jin, Yingdi; Hu, Xiangqian; Hu, Hao
2013-09-10
Accurate computation of the pKa value of a compound in solution is important but challenging. Here, a new mixing quantum mechanical/molecular mechanical (QM/MM) Hamiltonian method is developed to simulate the free-energy change associated with the protonation/deprotonation processes in solution. The mixing Hamiltonian method is designed for efficient quantum mechanical free-energy simulations by alchemically varying the nuclear potential, i.e., the nuclear charge of the transforming nucleus. In pKa calculation, the charge on the proton is varied in fraction between 0 and 1, corresponding to the fully deprotonated and protonated states, respectively. Inspired by the mixing potential QM/MM free energy simulation method developed previously [H. Hu and W. T. Yang, J. Chem. Phys. 2005, 123, 041102], this method succeeds many advantages of a large class of λ-coupled free-energy simulation methods and the linear combination of atomic potential approach. Theory and technique details of this method, along with the calculation results of the pKa of methanol and methanethiol molecules in aqueous solution, are reported. The results show satisfactory agreement with the experimental data.
International Nuclear Information System (INIS)
Sehrawat, Arun; Englert, Berthold-Georg; Zemann, Daniel
2011-01-01
We present a hybrid model of the unitary-evolution-based quantum computation model and the measurement-based quantum computation model. In the hybrid model, part of a quantum circuit is simulated by unitary evolution and the rest by measurements on star graph states, thereby combining the advantages of the two standard quantum computation models. In the hybrid model, a complicated unitary gate under simulation is decomposed in terms of a sequence of single-qubit operations, the controlled-z gates, and multiqubit rotations around the z axis. Every single-qubit and the controlled-z gate are realized by a respective unitary evolution, and every multiqubit rotation is executed by a single measurement on a required star graph state. The classical information processing in our model requires only an information flow vector and propagation matrices. We provide the implementation of multicontrol gates in the hybrid model. They are very useful for implementing Grover's search algorithm, which is studied as an illustrative example.
Lonsdale, Richard; Reetz, Manfred T
2015-11-25
Enoate reductases catalyze the reduction of activated C═C bonds with high enantioselectivity. The oxidative half-reaction, which involves the addition of a hydride and a proton to opposite faces of the C═C bond, has been studied for the first time by hybrid quantum mechanics/molecular mechanics (QM/MM). The reduction of 2-cyclohexen-1-one by YqjM from Bacillus subtilis was selected as the model system. Two-dimensional QM/MM (B3LYP-D/OPLS2005) reaction pathways suggest that the hydride and proton are added as distinct steps, with the former step preceding the latter. Furthermore, we present interesting insights into the reactivity of this enzyme, including the weak binding of the substrate in the active site, the role of the two active site histidine residues for polarization of the substrate C═O bond, structural details of the transition states to hydride and proton transfer, and the role of Tyr196 as proton donor. The information presented here will be useful for the future design of enantioselective YqjM mutants for other substrates.
Lonsdale, Richard; Fort, Rachel M; Rydberg, Patrik; Harvey, Jeremy N; Mulholland, Adrian J
2016-06-20
The mechanism of cytochrome P450(CYP)-catalyzed hydroxylation of primary amines is currently unclear and is relevant to drug metabolism; previous small model calculations have suggested two possible mechanisms: direct N-oxidation and H-abstraction/rebound. We have modeled the N-hydroxylation of (R)-mexiletine in CYP1A2 with hybrid quantum mechanics/molecular mechanics (QM/MM) methods, providing a more detailed and realistic model. Multiple reaction barriers have been calculated at the QM(B3LYP-D)/MM(CHARMM27) level for the direct N-oxidation and H-abstraction/rebound mechanisms. Our calculated barriers indicate that the direct N-oxidation mechanism is preferred and proceeds via the doublet spin state of Compound I. Molecular dynamics simulations indicate that the presence of an ordered water molecule in the active site assists in the binding of mexiletine in the active site, but this is not a prerequisite for reaction via either mechanism. Several active site residues play a role in the binding of mexiletine in the active site, including Thr124 and Phe226. This work reveals key details of the N-hydroxylation of mexiletine and further demonstrates that mechanistic studies using QM/MM methods are useful for understanding drug metabolism.
Mendieta-Moreno, Jesús I; Marcos-Alcalde, Iñigo; Trabada, Daniel G; Gómez-Puertas, Paulino; Ortega, José; Mendieta, Jesús
2015-01-01
Quantum mechanics/molecular mechanics (QM/MM) methods are excellent tools for the modeling of biomolecular reactions. Recently, we have implemented a new QM/MM method (Fireball/Amber), which combines an efficient density functional theory method (Fireball) and a well-recognized molecular dynamics package (Amber), offering an excellent balance between accuracy and sampling capabilities. Here, we present a detailed explanation of the Fireball method and Fireball/Amber implementation. We also discuss how this tool can be used to analyze reactions in biomolecules using steered molecular dynamics simulations. The potential of this approach is shown by the analysis of a reaction catalyzed by the enzyme triose-phosphate isomerase (TIM). The conformational space and energetic landscape for this reaction are analyzed without a priori assumptions about the protonation states of the different residues during the reaction. The results offer a detailed description of the reaction and reveal some new features of the catalytic mechanism. In particular, we find a new reaction mechanism that is characterized by the intramolecular proton transfer from O1 to O2 and the simultaneous proton transfer from Glu 165 to C2. Copyright © 2015 Elsevier Inc. All rights reserved.
Quantum Mechanics/Molecular Mechanics Modeling of Enzymatic Processes: Caveats and Breakthroughs.
Quesne, Matthew G; Borowski, Tomasz; de Visser, Sam P
2016-02-18
Nature has developed large groups of enzymatic catalysts with the aim to transfer substrates into useful products, which enables biosystems to perform all their natural functions. As such, all biochemical processes in our body (we drink, we eat, we breath, we sleep, etc.) are governed by enzymes. One of the problems associated with research on biocatalysts is that they react so fast that details of their reaction mechanisms cannot be obtained with experimental work. In recent years, major advances in computational hardware and software have been made and now large (bio)chemical systems can be studied using accurate computational techniques. One such technique is the quantum mechanics/molecular mechanics (QM/MM) technique, which has gained major momentum in recent years. Unfortunately, it is not a black-box method that is easily applied, but requires careful set-up procedures. In this work we give an overview on the technical difficulties and caveats of QM/MM and discuss work-protocols developed in our groups for running successful QM/MM calculations. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Moreira, Cátia; Ramos, Maria J; Fernandes, Pedro Alexandrino
2016-06-27
This paper is devoted to the understanding of the reaction mechanism of mycobacterium tuberculosis glutamine synthetase (mtGS) with atomic detail, using computational quantum mechanics/molecular mechanics (QM/MM) methods at the ONIOM M06-D3/6-311++G(2d,2p):ff99SB//B3LYP/6-31G(d):ff99SB level of theory. The complete reaction undergoes a three-step mechanism: the spontaneous transfer of phosphate from ATP to glutamate upon ammonium binding (ammonium quickly loses a proton to Asp54), the attack of ammonia on phosphorylated glutamate (yielding protonated glutamine), and the deprotonation of glutamine by the leaving phosphate. This exothermic reaction has an activation free energy of 21.5 kcal mol(-1) , which is consistent with that described for Escherichia coli glutamine synthetase (15-17 kcal mol(-1) ). The participating active site residues have been identified and their role and energy contributions clarified. This study provides an insightful atomic description of the biosynthetic reaction that takes place in this enzyme, opening doors for more accurate studies for developing new anti-tuberculosis therapies. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Jitonnom, Jitrayut; Mujika, Jon I; van der Kamp, Marc W; Mulholland, Adrian J
2017-12-05
Creatininase catalyzes the conversion of creatinine (a biosensor for kidney function) to creatine via a two-step mechanism: water addition followed by ring opening. Water addition is common to other known cyclic amidohydrolases, but the precise mechanism for ring opening is still under debate. The proton donor in this step is either His178 or a water molecule bound to one of the metal ions, and the roles of His178 and Glu122 are unclear. Here, the two possible reaction pathways have been fully examined by means of combined quantum mechanics/molecular mechanics simulations at the SCC-DFTB/CHARMM22 level of theory. The results indicate that His178 is the main catalytic residue for the whole reaction and explain its role as proton shuttle during the ring-opening step. In the first step, His178 provides electrostatic stabilization to the gem-diolate tetrahedral intermediate. In the second step, His178 abstracts the hydroxyl proton of the intermediate and delivers it to the cyclic amide nitrogen, leading to ring opening. The latter is the rate-limiting step with a free energy barrier of 18.5 kcal/mol, in agreement with the experiment. We find that Glu122 must be protonated during the enzyme reaction, so that it can form a stable hydrogen bond with its neighboring water molecule. Simulations of the E122Q mutant showed that this replacement disrupts the H-bond network formed by three conserved residues (Glu34, Ser78, and Glu122) and water, increasing the energy barrier. Our computational studies provide a comprehensive explanation for previous structural and kinetic observations, including why the H178A mutation causes a complete loss of activity but the E122Q mutation does not.
DEFF Research Database (Denmark)
Steinmann, Casper; Olsen, Jógvan Magnus Haugaard; Kongsted, Jacob
2014-01-01
We present NMR shielding constants obtained through quantum mechanical/molecular mechanical (QM/MM) embedding calculations. Contrary to previous reports, we show that a relatively small QM region is sufficient, provided that a high-quality embedding potential is used. The calculated averaged NMR...... shielding constants of both acrolein and acetone solvated in water are based on a number of snapshots extracted from classical molecular dynamics simulations. We focus on the carbonyl chromophore in both molecules, which shows large solvation effects, and we study the convergence of shielding constants...
Tvaroška, Igor
2015-02-11
Glycosyltransferases catalyze the formation of glycosidic bonds by assisting the transfer of a sugar residue from donors to specific acceptor molecules. Although structural and kinetic data have provided insight into mechanistic strategies employed by these enzymes, molecular modeling studies are essential for the understanding of glycosyltransferase catalyzed reactions at the atomistic level. For such modeling, combined quantum mechanics/molecular mechanics (QM/MM) methods have emerged as crucial. These methods allow the modeling of enzymatic reactions by using quantum mechanical methods for the calculation of the electronic structure of the active site models and treating the remaining enzyme environment by faster molecular mechanics methods. Herein, the application of QM/MM methods to glycosyltransferase catalyzed reactions is reviewed, and the insight from modeling of glycosyl transfer into the mechanisms and transition states structures of both inverting and retaining glycosyltransferases are discussed. Copyright © 2014 Elsevier Ltd. All rights reserved.
Álvarez-Barcia, Sonia; Kästner, Johannes
2017-06-01
Taurine/α-ketoglutarate dioxygenase is one of the most studied α-ketoglutarate-dependent dioxygenases (αKGDs), involved in several biotechnological applications. We investigated the key step in the catalytic cycle of the αKGDs, the hydrogen transfer process, by a quantum mechanics/molecular mechanics approach (B3LYP/CHARMM22). Analysis of the charge and spin densities during the reaction demonstrates that a concerted mechanism takes place, where the H atom transfer happens simultaneously with the electron transfer from taurine to the Fe═O cofactor. We found the quantum tunneling of the hydrogen atom to increase the rate constant by a factor of 40 at 5 °C. As a consequence, a quite high kinetic isotope effect close to 60 is obtained, which is consistent with the experimental value.
Zhu, Kongkai; Lu, Junyan; Liang, Zhongjie; Kong, Xiangqian; Ye, Fei; Jin, Lu; Geng, Heji; Chen, Yong; Zheng, Mingyue; Jiang, Hualiang; Li, Jun-Qian; Luo, Cheng
2013-03-01
New Delhi metallo-β-lactamase-1 (NDM-1) has emerged as a major global threat to human health for its rapid rate of dissemination and ability to make pathogenic microbes resistant to almost all known β-lactam antibiotics. In addition, effective NDM-1 inhibitors have not been identified to date. In spite of the plethora of structural and kinetic data available, the accurate molecular characteristics of and details on the enzymatic reaction of NDM-1 hydrolyzing β-lactam antibiotics remain incompletely understood. In this study, a combined computational approach including molecular docking, molecular dynamics simulations and quantum mechanics/molecular mechanics calculations was performed to characterize the catalytic mechanism of meropenem catalyzed by NDM-1. The quantum mechanics/molecular mechanics results indicate that the ionized D124 is beneficial to the cleavage of the C-N bond within the β-lactam ring. Meanwhile, it is energetically favorable to form an intermediate if no water molecule coordinates to Zn2. Moreover, according to the molecular dynamics results, the conserved residue K211 plays a pivotal role in substrate binding and catalysis, which is quite consistent with previous mutagenesis data. Our study provides detailed insights into the catalytic mechanism of NDM-1 hydrolyzing meropenem β-lactam antibiotics and offers clues for the discovery of new antibiotics against NDM-1 positive strains in clinical studies.
Watanabe, Hiroshi C; Banno, Misa; Sakurai, Minoru
2016-03-14
Quantum effects in solute-solvent interactions, such as the many-body effect and the dipole-induced dipole, are known to be critical factors influencing the infrared spectra of species in the liquid phase. For accurate spectrum evaluation, the surrounding solvent molecules, in addition to the solute of interest, should be treated using a quantum mechanical method. However, conventional quantum mechanics/molecular mechanics (QM/MM) methods cannot handle free QM solvent molecules during molecular dynamics (MD) simulation because of the diffusion problem. To deal with this problem, we have previously proposed an adaptive QM/MM "size-consistent multipartitioning (SCMP) method". In the present study, as the first application of the SCMP method, we demonstrate the reproduction of the infrared spectrum of liquid-phase water, and evaluate the quantum effect in comparison with conventional QM/MM simulations.
Quantum technologies with hybrid systems
Kurizki, Gershon; Bertet, Patrice; Kubo, Yuimaru; Mølmer, Klaus; Petrosyan, David; Rabl, Peter; Schmiedmayer, Jörg
2015-03-01
An extensively pursued current direction of research in physics aims at the development of practical technologies that exploit the effects of quantum mechanics. As part of this ongoing effort, devices for quantum information processing, secure communication, and high-precision sensing are being implemented with diverse systems, ranging from photons, atoms, and spins to mesoscopic superconducting and nanomechanical structures. Their physical properties make some of these systems better suited than others for specific tasks; thus, photons are well suited for transmitting quantum information, weakly interacting spins can serve as long-lived quantum memories, and superconducting elements can rapidly process information encoded in their quantum states. A central goal of the envisaged quantum technologies is to develop devices that can simultaneously perform several of these tasks, namely, reliably store, process, and transmit quantum information. Hybrid quantum systems composed of different physical components with complementary functionalities may provide precisely such multitasking capabilities. This article reviews some of the driving theoretical ideas and first experimental realizations of hybrid quantum systems and the opportunities and challenges they present and offers a glance at the near- and long-term perspectives of this fascinating and rapidly expanding field.
Quantum technologies with hybrid systems
Kurizki, Gershon; Bertet, Patrice; Kubo, Yuimaru; Mølmer, Klaus; Petrosyan, David; Rabl, Peter; Schmiedmayer, Jörg
2015-01-01
An extensively pursued current direction of research in physics aims at the development of practical technologies that exploit the effects of quantum mechanics. As part of this ongoing effort, devices for quantum information processing, secure communication, and high-precision sensing are being implemented with diverse systems, ranging from photons, atoms, and spins to mesoscopic superconducting and nanomechanical structures. Their physical properties make some of these systems better suited than others for specific tasks; thus, photons are well suited for transmitting quantum information, weakly interacting spins can serve as long-lived quantum memories, and superconducting elements can rapidly process information encoded in their quantum states. A central goal of the envisaged quantum technologies is to develop devices that can simultaneously perform several of these tasks, namely, reliably store, process, and transmit quantum information. Hybrid quantum systems composed of different physical components with complementary functionalities may provide precisely such multitasking capabilities. This article reviews some of the driving theoretical ideas and first experimental realizations of hybrid quantum systems and the opportunities and challenges they present and offers a glance at the near- and long-term perspectives of this fascinating and rapidly expanding field. PMID:25737558
Quantum technologies with hybrid systems.
Kurizki, Gershon; Bertet, Patrice; Kubo, Yuimaru; Mølmer, Klaus; Petrosyan, David; Rabl, Peter; Schmiedmayer, Jörg
2015-03-31
An extensively pursued current direction of research in physics aims at the development of practical technologies that exploit the effects of quantum mechanics. As part of this ongoing effort, devices for quantum information processing, secure communication, and high-precision sensing are being implemented with diverse systems, ranging from photons, atoms, and spins to mesoscopic superconducting and nanomechanical structures. Their physical properties make some of these systems better suited than others for specific tasks; thus, photons are well suited for transmitting quantum information, weakly interacting spins can serve as long-lived quantum memories, and superconducting elements can rapidly process information encoded in their quantum states. A central goal of the envisaged quantum technologies is to develop devices that can simultaneously perform several of these tasks, namely, reliably store, process, and transmit quantum information. Hybrid quantum systems composed of different physical components with complementary functionalities may provide precisely such multitasking capabilities. This article reviews some of the driving theoretical ideas and first experimental realizations of hybrid quantum systems and the opportunities and challenges they present and offers a glance at the near- and long-term perspectives of this fascinating and rapidly expanding field.
Hybrid quantum-classical master equations
International Nuclear Information System (INIS)
Diósi, Lajos
2014-01-01
We discuss hybrid master equations of composite systems, which are hybrids of classical and quantum subsystems. A fairly general form of hybrid master equations is suggested. Its consistency is derived from the consistency of Lindblad quantum master equations. We emphasize that quantum measurement is a natural example of exact hybrid systems. We derive a heuristic hybrid master equation of time-continuous position measurement (monitoring). (paper)
Mondal, Padmabati; Granucci, Giovanni; Rastädter, Dominique; Persico, Maurizio; Burghardt, Irene
2018-05-28
The photoregulation of nucleic acids by azobenzene photoswitches has recently attracted considerable interest in the context of emerging biotechnological applications. To understand the mechanism of photoinduced isomerisation and conformational control in these complex biological environments, we employ a Quantum Mechanics/Molecular Mechanics (QM/MM) approach in conjunction with nonadiabatic Surface Hopping (SH) dynamics. Two representative RNA-azobenzene complexes are investigated, both of which contain the azobenzene chromophore covalently attached to an RNA double strand via a β-deoxyribose linker. Due to the pronounced constraints of the local RNA environment, it is found that trans -to- cis isomerization is slowed down to a time scale of ∼10-15 picoseconds, in contrast to 500 femtoseconds in vacuo , with a quantum yield reduced by a factor of two. By contrast, cis -to- trans isomerization remains in a sub-picosecond regime. A volume-conserving isomerization mechanism is found, similarly to the pedal-like mechanism previously identified for azobenzene in solution phase. Strikingly, the chiral RNA environment induces opposite right-handed and left-handed helicities of the ground-state cis -azobenzene chromophore in the two RNA-azobenzene complexes, along with an almost completely chirality conserving photochemical pathway for these helical enantiomers.
Sodt, Alexander J; Mei, Ye; König, Gerhard; Tao, Peng; Steele, Ryan P; Brooks, Bernard R; Shao, Yihan
2015-03-05
In combined quantum mechanical/molecular mechanical (QM/MM) free energy calculations, it is often advantageous to have a frozen geometry for the quantum mechanical (QM) region. For such multiple-environment single-system (MESS) cases, two schemes are proposed here for estimating the polarization energy: the first scheme, termed MESS-E, involves a Roothaan step extrapolation of the self-consistent field (SCF) energy; whereas the other scheme, termed MESS-H, employs a Newton-Raphson correction using an approximate inverse electronic Hessian of the QM region (which is constructed only once). Both schemes are extremely efficient, because the expensive Fock updates and SCF iterations in standard QM/MM calculations are completely avoided at each configuration. They produce reasonably accurate QM/MM polarization energies: MESS-E can predict the polarization energy within 0.25 kcal/mol in terms of the mean signed error for two of our test cases, solvated methanol and solvated β-alanine, using the M06-2X or ωB97X-D functionals; MESS-H can reproduce the polarization energy within 0.2 kcal/mol for these two cases and for the oxyluciferin-luciferase complex, if the approximate inverse electronic Hessians are constructed with sufficient accuracy.
Shen, Lin; Yang, Weitao
2018-03-13
Direct molecular dynamics (MD) simulation with ab initio quantum mechanical and molecular mechanical (QM/MM) methods is very powerful for studying the mechanism of chemical reactions in a complex environment but also very time-consuming. The computational cost of QM/MM calculations during MD simulations can be reduced significantly using semiempirical QM/MM methods with lower accuracy. To achieve higher accuracy at the ab initio QM/MM level, a correction on the existing semiempirical QM/MM model is an attractive idea. Recently, we reported a neural network (NN) method as QM/MM-NN to predict the potential energy difference between semiempirical and ab initio QM/MM approaches. The high-level results can be obtained using neural network based on semiempirical QM/MM MD simulations, but the lack of direct MD samplings at the ab initio QM/MM level is still a deficiency that limits the applications of QM/MM-NN. In the present paper, we developed a dynamic scheme of QM/MM-NN for direct MD simulations on the NN-predicted potential energy surface to approximate ab initio QM/MM MD. Since some configurations excluded from the database for NN training were encountered during simulations, which may cause some difficulties on MD samplings, an adaptive procedure inspired by the selection scheme reported by Behler [ Behler Int. J. Quantum Chem. 2015 , 115 , 1032 ; Behler Angew. Chem., Int. Ed. 2017 , 56 , 12828 ] was employed with some adaptions to update NN and carry out MD iteratively. We further applied the adaptive QM/MM-NN MD method to the free energy calculation and transition path optimization on chemical reactions in water. The results at the ab initio QM/MM level can be well reproduced using this method after 2-4 iteration cycles. The saving in computational cost is about 2 orders of magnitude. It demonstrates that the QM/MM-NN with direct MD simulations has great potentials not only for the calculation of thermodynamic properties but also for the characterization of
Capoferri, Luigi; Lodola, Alessio; Rivara, Silvia; Mor, Marco
2015-03-23
Irreversible epidermal growth factor receptor (EGFR) inhibitors can circumvent resistance to first-generation ATP-competitive inhibitors in the treatment of nonsmall-cell lung cancer. They covalently bind a noncatalytic cysteine (Cys797) at the surface of EGFR active site by an acrylamide warhead. Herein, we used a hybrid quantum mechanics/molecular mechanics (QM/MM) potential in combination with umbrella sampling in the path-collective variable space to investigate the mechanism of alkylation of Cys797 by the prototypical covalent inhibitor N-(4-anilinoquinazolin-6-yl) acrylamide. Calculations show that Cys797 reacts with the acrylamide group of the inhibitor through a direct addition mechanism, with Asp800 acting as a general base/general acid in distinct steps of the reaction. The obtained reaction free energy is negative (ΔA = -12 kcal/mol) consistent with the spontaneous and irreversible alkylation of Cys797 by N-(4-anilinoquinazolin-6-yl) acrylamide. Our calculations identify desolvation of Cys797 thiolate anion as a key step of the alkylation process, indicating that changes in the intrinsic reactivity of the acrylamide would have only a minor impact on the inhibitor potency.
Directory of Open Access Journals (Sweden)
James W. Gauld
2012-10-01
Full Text Available Ornithine cyclodeaminase (OCD is an NAD+-dependent deaminase that is found in bacterial species such as Pseudomonas putida. Importantly, it catalyzes the direct conversion of the amino acid L-ornithine to L-proline. Using molecular dynamics (MD and a hybrid quantum mechanics/molecular mechanics (QM/MM method in the ONIOM formalism, the catalytic mechanism of OCD has been examined. The rate limiting step is calculated to be the initial step in the overall mechanism: hydride transfer from the L-ornithine’s Cα–H group to the NAD+ cofactor with concomitant formation of a Cα=NH2+ Schiff base with a barrier of 90.6 kJ mol−1. Importantly, no water is observed within the active site during the MD simulations suitably positioned to hydrolyze the Cα=NH2+ intermediate to form the corresponding carbonyl. Instead, the reaction proceeds via a non-hydrolytic mechanism involving direct nucleophilic attack of the δ-amine at the Cα-position. This is then followed by cleavage and loss of the α-NH2 group to give the Δ1-pyrroline-2-carboxylate that is subsequently reduced to L-proline.
Löytynoja, T; Niskanen, J; Jänkälä, K; Vahtras, O; Rinkevicius, Z; Ågren, H
2014-11-20
Using ethanol-water solutions as illustration, we demonstrate the capability of the hybrid quantum mechanics/molecular mechanics (QM/MM) paradigm to simulate core photoelectron spectroscopy: the binding energies and the chemical shifts. An integrated approach with QM/MM binding energy calculations coupled to preceding molecular dynamics sampling is adopted to generate binding energies averaged over the solute-solvent configurations available at a particular temperature and pressure and thus allowing for a statistical assessment with confidence levels for the final binding energies. The results are analyzed in terms of the contributions in the molecular mechanics model-electrostatic, polarization, and van der Waals-with atom or bond granulation of the corresponding MM charge and polarizability force-fields. The role of extramolecular charge transfer screening of the core-hole and explicit hydrogen bonding is studied by extending the QM core to cover the first solvation shell. The results are compared to those obtained from pure electrostatic and polarizable continuum models. Particularly, the dependence of the carbon 1s binding energies with respect to the ethanol concentration is studied. Our results indicate that QM/MM can be used as an all-encompassing model to study photoelectron binding energies and chemical shifts in solvent environments.
Ha, Nguyen Ngoc; Cam, Le Minh; Ha, Nguyen Thi Thu; Goh, Bee-Min; Saunders, Martin; Jiang, Zhong-Tao; Altarawneh, Mohammednoor; Dlugogorski, Bogdan Z; El-Harbawi, Mohanad; Yin, Chun-Yang
2017-06-07
The prevalence of global arsenic groundwater contamination has driven widespread research on developing effective treatment systems including adsorption using various sorbents. The uptake of arsenic-based contaminants onto established sorbents such as activated carbon (AC) can be effectively enhanced via immobilization/impregnation of iron-based elements on the porous AC surface. Recent suggestions that AC pores structurally consist of an eclectic mix of curved fullerene-like sheets may affect the arsenic adsorption dynamics within the AC pores and is further complicated by the presence of nano-sized iron-based elements. We have therefore, attempted to shed light on the adsorptive interactions of arsenate-iron nanoparticles with curved fullerene-like sheets by using hybridized quantum mechanics/molecular mechanics (QMMM) calculations and microscopy characterization. It is found that, subsequent to optimization, chemisorption between HAsO 4 2- and the AC carbon sheet (endothermic process) is virtually non-existent - this observation is supported by experimental results. Conversely, the incorporation of iron nanoparticles (FeNPs) into the AC carbon sheet greatly facilitates chemisorption of HAsO 4 2- . Our calculation implies that iron carbide is formed at the junction between the iron and the AC interface and this tightly chemosorbed layer prevents detachment of the FeNPs on the AC surface. Other aspects including electronic structure/properties, carbon arrangement defects and rate of adsorptive interaction, which are determined using the Climbing-Image NEB method, are also discussed.
Ion, Bogdan F.; Bushnell, Eric A. C.; De Luna, Phil; Gauld, James W.
2012-01-01
Ornithine cyclodeaminase (OCD) is an NAD+-dependent deaminase that is found in bacterial species such as Pseudomonas putida. Importantly, it catalyzes the direct conversion of the amino acid L-ornithine to L-proline. Using molecular dynamics (MD) and a hybrid quantum mechanics/molecular mechanics (QM/MM) method in the ONIOM formalism, the catalytic mechanism of OCD has been examined. The rate limiting step is calculated to be the initial step in the overall mechanism: hydride transfer from the L-ornithine’s Cα–H group to the NAD+ cofactor with concomitant formation of a Cα=NH2 + Schiff base with a barrier of 90.6 kJ mol−1. Importantly, no water is observed within the active site during the MD simulations suitably positioned to hydrolyze the Cα=NH2 + intermediate to form the corresponding carbonyl. Instead, the reaction proceeds via a non-hydrolytic mechanism involving direct nucleophilic attack of the δ-amine at the Cα-position. This is then followed by cleavage and loss of the α-NH2 group to give the Δ1-pyrroline-2-carboxylate that is subsequently reduced to L-proline. PMID:23202934
Duster, Adam W; Lin, Hai
2017-09-14
Recently, a collective variable "proton indicator" was purposed for tracking an excess proton solvated in bulk water in molecular dynamics simulations. In this work, we demonstrate the feasibility of utilizing the position of this proton indicator as a reaction coordinate to model an excess proton migrating through a hydrophobic carbon nanotube in combined quantum-mechanics/molecular-mechanics simulations. Our results indicate that applying a harmonic restraint to the proton indicator in the bulk solvent near the nanotube pore entrance leads to the recruitment of water molecules into the pore. This is consistent with an earlier study that employed a multistate empirical valence bond potential and a different representation (center of excess charge) of the proton. We attribute this water recruitment to the delocalized nature of the solvated proton, which prefers to be in high-dielectric bulk solvent. While water recruitment into the pore is considered an artifact in the present simulations (because of the artificially imposed restraint on the proton), if the proton were naturally restrained, it could assist in building water wires prior to proton transfer through the pore. The potential of mean force for a proton translocation through the water-filled pore was computed by umbrella sampling, where the bias potentials were applied to the proton indicator. The free energy curve and barrier heights agree reasonably with those in the literature. The results suggest that the proton indicator can be used as a reaction coordinate in simulations of proton transport in confined environments.
Zhang, Ruiming; Shi, Xiangli; Sun, Yanhui; Zhang, Qingzhu; Wang, Wenxing
2018-05-17
The present study delineated the dehydrogenation mechanism of cis-2,3-dihydro-2,3-dihydroxybiphenyl (2,3-DDBPH) and cis-2,3-dihydro-2,3-dihydroxy-4,4'-dichlorobiphenyl (2,3-DD-4,4'-DBPH) by Pandoraea pnomenusa strain B-356 cis-2,3-dihydro-2,3-dihydroxybiphenyl dehydrogenase (BphB) in atomistic detail. The enzymatic process was investigated by a combined quantum mechanics/molecular mechanics (QM/MM) approach. Five different snapshots were extracted and calculated, which revealed that the Boltzmann-weighted average barriers of 2,3-DDBPH and 2,3-DD-4,4'-DBPH dehydrogenation processes are 10.7 and 11.5 kcal mol -1 , respectively. The established dehydrogenation mechanism provides new insight into the degradation processes of other chlorinated 2,3-DDBPH. In addition to Asn115, Ser142, and Lys149, the importance of Ile 89, Asn143, Pro184, Met 187, Thr189, and Lue 191 during the dehydrogenation process of 2,3-DDBPH and 2,3-DD-4,4'-DBPH were also highlighted to search for promising mutation targets for improving the catalytic efficiency of BphB. Copyright © 2018. Published by Elsevier Ltd.
Xu, Yulong; Zhang, Jingxue; Wang, Dunyou
2015-06-28
The CH3Cl + CN(-) reaction in water was studied using a multilevel quantum mechanics/molecular mechanics (MM) method with the multilevels, electrostatic potential, density functional theory (DFT) and coupled-cluster single double triple (CCSD(T)), for the solute region. The detailed, back-side attack SN2 reaction mechanism was mapped along the reaction pathway. The potentials of mean force were calculated under both the DFT and CCSD(T) levels for the reaction region. The CCSD(T)/MM level of theory presents a free energy activation barrier height at 20.3 kcal/mol, which agrees very well with the experiment value at 21.6 kcal/mol. The results show that the aqueous solution has a dominant role in shaping the potential of mean force. The solvation effect and the polarization effect together increase the activation barrier height by ∼11.4 kcal/mol: the solvation effect plays a major role by providing about 75% of the contribution, while polarization effect only contributes 25% to the activation barrier height. Our calculated potential of mean force under the CCSD(T)/MM also has a good agreement with the one estimated using data from previous gas-phase studies.
International Nuclear Information System (INIS)
Zeng Xiancheng; Hu Hao; Hu Xiangqian; Yang Weitao
2009-01-01
A quantum mechanical/molecular mechanical minimum free energy path (QM/MM-MFEP) method was developed to calculate the redox free energies of large systems in solution with greatly enhanced efficiency for conformation sampling. The QM/MM-MFEP method describes the thermodynamics of a system on the potential of mean force surface of the solute degrees of freedom. The molecular dynamics (MD) sampling is only carried out with the QM subsystem fixed. It thus avoids 'on-the-fly' QM calculations and thus overcomes the high computational cost in the direct QM/MM MD sampling. In the applications to two metal complexes in aqueous solution, the new QM/MM-MFEP method yielded redox free energies in good agreement with those calculated from the direct QM/MM MD method. Two larger biologically important redox molecules, lumichrome and riboflavin, were further investigated to demonstrate the efficiency of the method. The enhanced efficiency and uncompromised accuracy are especially significant for biochemical systems. The QM/MM-MFEP method thus provides an efficient approach to free energy simulation of complex electron transfer reactions.
Nauton, Lionel; Hélaine, Virgil; Théry, Vincent; Hecquet, Laurence
2016-04-12
We propose the first computational model for transketolase (TK), a thiamine diphosphate (ThDP)-dependent enzyme, using a quantum mechanical/molecular mechanical method on the basis of crystallographic TK structures from yeast and Escherichia coli, together with experimental kinetic data reported in the literature with wild-type and mutant TK. This model allowed us to define a new route for ThDP activation in the enzyme environment. We evidenced a strong interaction between ThDP and Glu418B of the TK active site, itself stabilized by Glu162A. The crucial point highlighted here is that deprotonation of ThDP C2 is not performed by ThDP N4' as reported in the literature, but by His481B, involving a HOH688A molecule bridge. Thus, ThDP N4' is converted from an amino form to an iminium form, ensuring the stabilization of the C2 carbanion or carbene. Finally, ThDP activation proceeds via an intermolecular process and not by an intramolecular one as reported in the literature. More generally, this proposed ThDP activation mechanism can be applied to some other ThDP-dependent enzymes and used to define the entire TK mechanism with donor and acceptor substrates more accurately.
König, Gerhard; Mei, Ye; Pickard, Frank C; Simmonett, Andrew C; Miller, Benjamin T; Herbert, John M; Woodcock, H Lee; Brooks, Bernard R; Shao, Yihan
2016-01-12
A recently developed MESS-E-QM/MM method (multiple-environment single-system quantum mechanical molecular/mechanical calculations with a Roothaan-step extrapolation) is applied to the computation of hydration free energies for the blind SAMPL4 test set and for 12 small molecules. First, free energy simulations are performed with a classical molecular mechanics force field using fixed-geometry solute molecules and explicit TIP3P solvent, and then the non-Boltzmann-Bennett method is employed to compute the QM/MM correction (QM/MM-NBB) to the molecular mechanical hydration free energies. For the SAMPL4 set, MESS-E-QM/MM-NBB corrections to the hydration free energy can be obtained 2 or 3 orders of magnitude faster than fully converged QM/MM-NBB corrections, and, on average, the hydration free energies predicted with MESS-E-QM/MM-NBB fall within 0.10-0.20 kcal/mol of full-converged QM/MM-NBB results. Out of five density functionals (BLYP, B3LYP, PBE0, M06-2X, and ωB97X-D), the BLYP functional is found to be most compatible with the TIP3P solvent model and yields the most accurate hydration free energies against experimental values for solute molecules included in this study.
Qi, Yue; Lu, Jiarui; Lai, Wenzhen
2016-05-26
To elucidate the reaction mechanism of the ring cleavage of homogentisate by homogentisate dioxygenase, quantum mechanical/molecular mechanical (QM/MM) calculations were carried out by using two systems in different protonation states of the substrate C2 hydroxyl group. When the substrate C2 hydroxyl group is ionized (the ionized pathway), the superoxo attack on the substrate is the rate-limiting step in the catalytic cycle, with a barrier of 15.9 kcal/mol. Glu396 was found to play an important role in stabilizing the bridge species and its O-O cleavage product by donating a proton via a hydrogen-bonded water molecule. When the substrate C2 hydroxyl group is not ionized (the nonionized pathway), the O-O bond cleavage of the bridge species is the rate-limiting step, with a barrier of 15.3 kcal/mol. The QM/MM-optimized geometries for the dioxygen and alkylperoxo complexes using the nonionized model (for the C2 hydroxyl group) are in agreement with the experimental crystal structures, suggesting that the C2 hydroxyl group is more likely to be nonionized.
Muždalo, Anja; Saalfrank, Peter; Vreede, Jocelyne; Santer, Mark
2018-04-10
Azobenzene-based molecular photoswitches are becoming increasingly important for the development of photoresponsive, functional soft-matter material systems. Upon illumination with light, fast interconversion between a more stable trans and a metastable cis configuration can be established resulting in pronounced changes in conformation, dipole moment or hydrophobicity. A rational design of functional photosensitive molecules with embedded azo moieties requires a thorough understanding of isomerization mechanisms and rates, especially the thermally activated relaxation. For small azo derivatives considered in the gas phase or simple solvents, Eyring's classical transition state theory (TST) approach yields useful predictions for trends in activation energies or corresponding half-life times of the cis isomer. However, TST or improved theories cannot easily be applied when the azo moiety is part of a larger molecular complex or embedded into a heterogeneous environment, where a multitude of possible reaction pathways may exist. In these cases, only the sampling of an ensemble of dynamic reactive trajectories (transition path sampling, TPS) with explicit models of the environment may reveal the nature of the processes involved. In the present work we show how a TPS approach can conveniently be implemented for the phenomenon of relaxation-isomerization of azobenzenes starting with the simple examples of pure azobenzene and a push-pull derivative immersed in a polar (DMSO) and apolar (toluene) solvent. The latter are represented explicitly at a molecular mechanical (MM) and the azo moiety at a quantum mechanical (QM) level. We demonstrate for the push-pull azobenzene that path sampling in combination with the chosen QM/MM scheme produces the expected change in isomerization pathway from inversion to rotation in going from a low to a high permittivity (explicit) solvent model. We discuss the potential of the simulation procedure presented for comparative calculation of
Universal blind quantum computation for hybrid system
Huang, He-Liang; Bao, Wan-Su; Li, Tan; Li, Feng-Guang; Fu, Xiang-Qun; Zhang, Shuo; Zhang, Hai-Long; Wang, Xiang
2017-08-01
As progress on the development of building quantum computer continues to advance, first-generation practical quantum computers will be available for ordinary users in the cloud style similar to IBM's Quantum Experience nowadays. Clients can remotely access the quantum servers using some simple devices. In such a situation, it is of prime importance to keep the security of the client's information. Blind quantum computation protocols enable a client with limited quantum technology to delegate her quantum computation to a quantum server without leaking any privacy. To date, blind quantum computation has been considered only for an individual quantum system. However, practical universal quantum computer is likely to be a hybrid system. Here, we take the first step to construct a framework of blind quantum computation for the hybrid system, which provides a more feasible way for scalable blind quantum computation.
Watanabe, Hiroshi C; Kubillus, Maximilian; Kubař, Tomáš; Stach, Robert; Mizaikoff, Boris; Ishikita, Hiroshi
2017-07-21
In the condensed phase, quantum chemical properties such as many-body effects and intermolecular charge fluctuations are critical determinants of the solvation structure and dynamics. Thus, a quantum mechanical (QM) molecular description is required for both solute and solvent to incorporate these properties. However, it is challenging to conduct molecular dynamics (MD) simulations for condensed systems of sufficient scale when adapting QM potentials. To overcome this problem, we recently developed the size-consistent multi-partitioning (SCMP) quantum mechanics/molecular mechanics (QM/MM) method and realized stable and accurate MD simulations, using the QM potential to a benchmark system. In the present study, as the first application of the SCMP method, we have investigated the structures and dynamics of Na + , K + , and Ca 2+ solutions based on nanosecond-scale sampling, a sampling 100-times longer than that of conventional QM-based samplings. Furthermore, we have evaluated two dynamic properties, the diffusion coefficient and difference spectra, with high statistical certainty. Furthermore the calculation of these properties has not previously been possible within the conventional QM/MM framework. Based on our analysis, we have quantitatively evaluated the quantum chemical solvation effects, which show distinct differences between the cations.
Quantum photonics hybrid integration platform
Energy Technology Data Exchange (ETDEWEB)
Murray, E.; Floether, F. F. [Cambridge Research Laboratory, Toshiba Research Europe Limited, 208 Science Park, Milton Road, Cambridge CB4 0GZ (United Kingdom); Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, Cambridge CB3 0HE (United Kingdom); Ellis, D. J. P.; Meany, T.; Bennett, A. J., E-mail: anthony.bennet@crl.toshiba.co.uk; Shields, A. J. [Cambridge Research Laboratory, Toshiba Research Europe Limited, 208 Science Park, Milton Road, Cambridge CB4 0GZ (United Kingdom); Lee, J. P. [Cambridge Research Laboratory, Toshiba Research Europe Limited, 208 Science Park, Milton Road, Cambridge CB4 0GZ (United Kingdom); Engineering Department, University of Cambridge, 9 J. J. Thomson Avenue, Cambridge CB3 0FA (United Kingdom); Griffiths, J. P.; Jones, G. A. C.; Farrer, I.; Ritchie, D. A. [Cavendish Laboratory, University of Cambridge, J.J. Thomson Avenue, Cambridge CB3 0HE (United Kingdom)
2015-10-26
Fundamental to integrated photonic quantum computing is an on-chip method for routing and modulating quantum light emission. We demonstrate a hybrid integration platform consisting of arbitrarily designed waveguide circuits and single-photon sources. InAs quantum dots (QD) embedded in GaAs are bonded to a SiON waveguide chip such that the QD emission is coupled to the waveguide mode. The waveguides are SiON core embedded in a SiO{sub 2} cladding. A tuneable Mach Zehnder interferometer (MZI) modulates the emission between two output ports and can act as a path-encoded qubit preparation device. The single-photon nature of the emission was verified using the on-chip MZI as a beamsplitter in a Hanbury Brown and Twiss measurement.
Directory of Open Access Journals (Sweden)
Sam P De Visser
2013-12-01
Full Text Available Cysteine protease enzymes are important for human physiology and catalyze key protein degradation pathways. These enzymes react via a nucleophilic reaction mechanism that involves a cysteine residue and the proton of a proximal histidine. Particularly efficient inhibitors of these enzymes are nitrile-based, however, the details of the catalytic reaction mechanism currently are poorly understood. To gain further insight into the inhibition of these molecules, we have performed a combined density functional theory and quantum mechanics/molecular mechanics study on the reaction of a nitrile-based inhibitor with the enzyme active site amino acids. We show here that small perturbations to the inhibitor structure can have dramatic effects on the catalysis and inhibition processes. Thus, we investigated a range of inhibitor templates and show that specific structural changes reduce the inhibitory efficiency by several orders of magnitude. Moreover, as the reaction takes place on a polar surface, we find strong differences between the DFT and QM/MM calculated energetics. In particular, the DFT model led to dramatic distortions from the starting structure and the convergence to a structure that would not fit the enzyme active site. In the subsequent QM/MM study we investigated the use of mechanical versus electronic embedding on the kinetics, thermodynamics and geometries along the reaction mechanism. We find minor effects on the kinetics of the reaction but large geometric and thermodynamics differences as a result of inclusion of electronic embedding corrections. The work here highlights the importance of model choice in the investigation of this biochemical reaction mechanism.
Li, Pengfei; Soudackov, Alexander V; Hammes-Schiffer, Sharon
2018-02-28
The proton-coupled electron transfer (PCET) reaction catalyzed by soybean lipoxygenase has served as a prototype for understanding hydrogen tunneling in enzymes. Herein this PCET reaction is studied with mixed quantum mechanical/molecular mechanical (QM/MM) free energy simulations. The free energy surfaces are computed as functions of the proton donor-acceptor (C-O) distance and the proton coordinate, and the potential of mean force is computed as a function of the C-O distance, inherently including anharmonicity. The simulation results are used to calculate the kinetic isotope effects for the wild-type enzyme (WT) and the L546A/L754A double mutant (DM), which have been measured experimentally to be ∼80 and ∼700, respectively. The PCET reaction is found to be exoergic for WT and slightly endoergic for the DM, and the equilibrium C-O distance for the reactant is found to be ∼0.2 Å greater for the DM than for WT. The larger equilibrium distance for the DM, which is due mainly to less optimal substrate binding in the expanded binding cavity, is primarily responsible for its higher kinetic isotope effect. The calculated potentials of mean force are anharmonic and relatively soft at shorter C-O distances, allowing efficient thermal sampling of the shorter distances required for effective hydrogen tunneling. The primarily local electrostatic field at the transferring hydrogen is ∼100 MV/cm in the direction to facilitate proton transfer and increases dramatically as the C-O distance decreases. These simulations suggest that the overall protein environment is important for conformational sampling of active substrate configurations aligned for proton transfer, but the PCET reaction is influenced primarily by local electrostatic effects that facilitate conformational sampling of shorter proton donor-acceptor distances required for effective hydrogen tunneling.
Le, Quang Anh Tuan; Kim, Seonghoon; Chang, Rakwoo; Kim, Yong Hwan
2015-07-30
Serum paraoxonase 1 (PON1) is a versatile enzyme for the hydrolysis of various substrates (e.g., lactones, phosphotriesters) and for the formation of a promising chemical platform γ-valerolactone. Elucidation of the PON1-catalyzed lactonase reaction mechanism is very important for understanding the enzyme function and for engineering this enzyme for specific applications. Kinetic study and hybrid quantum mechanics/molecular mechanics (QM/MM) method were used to investigate the PON1-catalyzed lactonase reaction of γ-butyrolactone (GBL) and (R)-γ-valerolactone (GVL). The activation energies obtained from the QM/MM calculations were in good agreement with the experiments. Interestingly, the QM/MM energy barriers at MP2/3-21G(d,p) level for the lactonase of GVL and GBL were respectively 14.3-16.2 and 11.5-13.1 kcal/mol, consistent with the experimental values (15.57 and 14.73 kcal/mol derived from respective kcat values of 36.62 and 147.21 s(-1)). The QM/MM energy barriers at MP2/6-31G(d) and MP2/6-31G(d,p) levels were also in relatively good agreements with the experiments. Importantly, the difference in the QM/MM energy barriers at MP2 level with all investigated basis sets for the lactonase of GVL and GBL were in excellent agreement with the experiments (0.9-3.1 and 0.8 kcal/mol, respectively). A detailed mechanism for the PON1-catalyzed lactonase reaction was also proposed in this study.
Optical hybrid quantum teleportation and its applications
Takeda, Shuntaro; Okada, Masanori; Furusawa, Akira
2017-08-01
Quantum teleportation, a transfer protocol of quantum states, is the essence of many sophisticated quantum information protocols. There have been two complementary approaches to optical quantum teleportation: discrete variables (DVs) and continuous variables (CVs). However, both approaches have pros and cons. Here we take a "hybrid" approach to overcome the current limitations: CV quantum teleportation of DVs. This approach enabled the first realization of deterministic quantum teleportation of photonic qubits without post-selection. We also applied the hybrid scheme to several experiments, including entanglement swapping between DVs and CVs, conditional CV teleportation of single photons, and CV teleportation of qutrits. We are now aiming at universal, scalable, and fault-tolerant quantum computing based on these hybrid technologies.
Das, Susanta; Nam, Kwangho; Major, Dan Thomas
2018-03-13
In recent years, a number of quantum mechanical-molecular mechanical (QM/MM) enzyme studies have investigated the dependence of reaction energetics on the size of the QM region using energy and free energy calculations. In this study, we revisit the question of QM region size dependence in QM/MM simulations within the context of energy and free energy calculations using a proton transfer in a DNA base pair as a test case. In the simulations, the QM region was treated with a dispersion-corrected AM1/d-PhoT Hamiltonian, which was developed to accurately describe phosphoryl and proton transfer reactions, in conjunction with an electrostatic embedding scheme using the particle-mesh Ewald summation method. With this rigorous QM/MM potential, we performed rather extensive QM/MM sampling, and found that the free energy reaction profiles converge rapidly with respect to the QM region size within ca. ±1 kcal/mol. This finding suggests that the strategy of QM/MM simulations with reasonably sized and selected QM regions, which has been employed for over four decades, is a valid approach for modeling complex biomolecular systems. We point to possible causes for the sensitivity of the energy and free energy calculations to the size of the QM region, and potential implications.
DEFF Research Database (Denmark)
Dohn, A. O.; Jónsson, E. Ö.; Levi, Gianluca
2017-01-01
A multiscale density functional theory-quantum mechanics/molecular mechanics (DFT-QM/MM) scheme is presented, based on an efficient electrostatic coupling between the electronic density obtained from a grid-based projector augmented wave (GPAW) implementation of density functional theory...... and a classical potential energy function. The scheme is implemented in a general fashion and can be used with various choices for the descriptions of the QM or MM regions. Tests on H2O clusters, ranging from dimer to decamer show that no systematic energy errors are introduced by the coupling that exceeds...
Kanaan, Natalia; Crehuet, Ramon; Imhof, Petra
2015-09-24
Base excision of mismatched or damaged nucleotides catalyzed by glycosylase enzymes is the first step of the base excision repair system, a machinery preserving the integrity of DNA. Thymine DNA glycosylase recognizes and removes mismatched thymine by cleaving the C1'-N1 bond between the base and the sugar ring. Our quantum mechanical/molecular mechanical calculations of this reaction in human thymine DNA glycosylase reveal a requirement for a positive charge in the active site to facilitate C1'-N1 bond scission: protonation of His151 significantly lowers the free energy barrier for C1'-N1 bond dissociation compared to the situation with neutral His151. Shuttling a proton from His151 to the thymine base further reduces the activation free energy for glycosidic bond cleavage. Classical molecular dynamics simulations of the H151A mutant suggest that the mutation to the smaller, neutral, residue increases the water accessibility of the thymine base, rendering direct proton transfer from the bulk feasible. Quantum mechanical/molecular mechanical calculations of the glycosidic bond cleavage reaction in the H151A mutant show that the activation free energy is slightly lower than in the wild-type enzyme, explaining the experimentally observed higher reaction rates in this mutant.
A Hybrid Chaotic Quantum Evolutionary Algorithm
DEFF Research Database (Denmark)
Cai, Y.; Zhang, M.; Cai, H.
2010-01-01
A hybrid chaotic quantum evolutionary algorithm is proposed to reduce amount of computation, speed up convergence and restrain premature phenomena of quantum evolutionary algorithm. The proposed algorithm adopts the chaotic initialization method to generate initial population which will form a pe...... tests. The presented algorithm is applied to urban traffic signal timing optimization and the effect is satisfied....
Hybrid Quantum-Classical Approach to Quantum Optimal Control.
Li, Jun; Yang, Xiaodong; Peng, Xinhua; Sun, Chang-Pu
2017-04-14
A central challenge in quantum computing is to identify more computational problems for which utilization of quantum resources can offer significant speedup. Here, we propose a hybrid quantum-classical scheme to tackle the quantum optimal control problem. We show that the most computationally demanding part of gradient-based algorithms, namely, computing the fitness function and its gradient for a control input, can be accomplished by the process of evolution and measurement on a quantum simulator. By posing queries to and receiving answers from the quantum simulator, classical computing devices update the control parameters until an optimal control solution is found. To demonstrate the quantum-classical scheme in experiment, we use a seven-qubit nuclear magnetic resonance system, on which we have succeeded in optimizing state preparation without involving classical computation of the large Hilbert space evolution.
Ferenczy, György G
2013-04-05
The application of the local basis equation (Ferenczy and Adams, J. Chem. Phys. 2009, 130, 134108) in mixed quantum mechanics/molecular mechanics (QM/MM) and quantum mechanics/quantum mechanics (QM/QM) methods is investigated. This equation is suitable to derive local basis nonorthogonal orbitals that minimize the energy of the system and it exhibits good convergence properties in a self-consistent field solution. These features make the equation appropriate to be used in mixed QM/MM and QM/QM methods to optimize orbitals in the field of frozen localized orbitals connecting the subsystems. Calculations performed for several properties in divers systems show that the method is robust with various choices of the frozen orbitals and frontier atom properties. With appropriate basis set assignment, it gives results equivalent with those of a related approach [G. G. Ferenczy previous paper in this issue] using the Huzinaga equation. Thus, the local basis equation can be used in mixed QM/MM methods with small size quantum subsystems to calculate properties in good agreement with reference Hartree-Fock-Roothaan results. It is shown that bond charges are not necessary when the local basis equation is applied, although they are required for the self-consistent field solution of the Huzinaga equation based method. Conversely, the deformation of the wave-function near to the boundary is observed without bond charges and this has a significant effect on deprotonation energies but a less pronounced effect when the total charge of the system is conserved. The local basis equation can also be used to define a two layer quantum system with nonorthogonal localized orbitals surrounding the central delocalized quantum subsystem. Copyright © 2013 Wiley Periodicals, Inc.
Hybrid quantum-classical modeling of quantum dot devices
Kantner, Markus; Mittnenzweig, Markus; Koprucki, Thomas
2017-11-01
The design of electrically driven quantum dot devices for quantum optical applications asks for modeling approaches combining classical device physics with quantum mechanics. We connect the well-established fields of semiclassical semiconductor transport theory and the theory of open quantum systems to meet this requirement. By coupling the van Roosbroeck system with a quantum master equation in Lindblad form, we introduce a new hybrid quantum-classical modeling approach, which provides a comprehensive description of quantum dot devices on multiple scales: it enables the calculation of quantum optical figures of merit and the spatially resolved simulation of the current flow in realistic semiconductor device geometries in a unified way. We construct the interface between both theories in such a way, that the resulting hybrid system obeys the fundamental axioms of (non)equilibrium thermodynamics. We show that our approach guarantees the conservation of charge, consistency with the thermodynamic equilibrium and the second law of thermodynamics. The feasibility of the approach is demonstrated by numerical simulations of an electrically driven single-photon source based on a single quantum dot in the stationary and transient operation regime.
Quantum state engineering in hybrid open quantum systems
Joshi, Chaitanya; Larson, Jonas; Spiller, Timothy P.
2016-04-01
We investigate a possibility to generate nonclassical states in light-matter coupled noisy quantum systems, namely, the anisotropic Rabi and Dicke models. In these hybrid quantum systems, a competing influence of coherent internal dynamics and environment-induced dissipation drives the system into nonequilibrium steady states (NESSs). Explicitly, for the anisotropic Rabi model, the steady state is given by an incoherent mixture of two states of opposite parities, but as each parity state displays light-matter entanglement, we also find that the full state is entangled. Furthermore, as a natural extension of the anisotropic Rabi model to an infinite spin subsystem, we next explored the NESS of the anisotropic Dicke model. The NESS of this linearized Dicke model is also an inseparable state of light and matter. With an aim to enrich the dynamics beyond the sustainable entanglement found for the NESS of these hybrid quantum systems, we also propose to combine an all-optical feedback strategy for quantum state protection and for establishing quantum control in these systems. Our present work further elucidates the relevance of such hybrid open quantum systems for potential applications in quantum architectures.
Sgrignani, Jacopo; Grazioso, Giovanni; De Amici, Marco
2016-09-13
The fast and constant development of drug resistant bacteria represents a serious medical emergency. To overcome this problem, the development of drugs with new structures and modes of action is urgently needed. In this work, we investigated, at the atomistic level, the mechanisms of hydrolysis of Meropenem by OXA-23, a class D β-lactamase, combining unbiased classical molecular dynamics and umbrella sampling simulations with classical force field-based and quantum mechanics/molecular mechanics potentials. Our calculations provide a detailed structural and dynamic picture of the molecular steps leading to the formation of the Meropenem-OXA-23 covalent adduct, the subsequent hydrolysis, and the final release of the inactive antibiotic. In this mechanistic framework, the predicted activation energy is in good agreement with experimental kinetic measurements, validating the expected reaction path.
Hybrid quantum systems: Outsourcing superconducting qubits
Cleland, Andrew
Superconducting qubits offer excellent prospects for manipulating quantum information, with good qubit lifetimes, high fidelity single- and two-qubit gates, and straightforward scalability (admittedly with multi-dimensional interconnect challenges). One interesting route for experimental development is the exploration of hybrid systems, i.e. coupling superconducting qubits to other systems. I will report on our group's efforts to develop approaches that will allow interfacing superconducting qubits in a quantum-coherent fashion to spin defects in solids, to optomechanical devices, and to resonant nanomechanical structures. The longer term goals of these efforts include transferring quantum states between different qubit systems; generating and receiving ``flying'' acoustic phonon-based as well as optical photon-based qubits; and ultimately developing systems that can be used for quantum memory, quantum computation and quantum communication, the last in both the microwave and fiber telecommunications bands. Work is supported by Grants from AFOSR, ARO, DOE and NSF.
Ridder, L.; Mulholland, A.J.; Rietjens, I.M.C.M.; Vervoort, J.
2000-01-01
A combined quantum mechanical and molecular mechanical (QM/MM) method (AM1/CHARMM) was used to investigate the mechanism of the aromatic hydroxylation of phenol by a flavin dependent phenol hydroxylase (PH), an essential reaction in the degradation of a wide range of aromatic compounds. The model
Quantum state engineering in hybrid open quantum systems
Joshi, Chaitanya; Larson, Jonas; Spiller, Timothy P.
2015-01-01
We investigate a possibility to generate nonclassical states in light-matter coupled noisy quantum systems, namely, the anisotropic Rabi and Dicke models. In these hybrid quantum systems, a competing influence of coherent internal dynamics and environment-induced dissipation drives the system into nonequilibrium steady states (NESSs). Explicitly, for the anisotropic Rabi model, the steady state is given by an incoherent mixture of two states of opposite parities, but as each parity state disp...
Hybrid quantum systems of ions and atoms
Sias, Carlo; Köhl, Michael
2014-01-01
In this chapter we review the progress in experiments with hybrid systems of trapped ions and ultracold neutral atoms. We give a theoretical overview over the atom-ion interactions in the cold regime and give a summary of the most important experimental results. We conclude with an overview of remaining open challenges and possible applications in hybrid quantum systems of ions and neutral atoms.
Silicon based quantum dot hybrid qubits
Kim, Dohun
2015-03-01
The charge and spin degrees of freedom of an electron constitute natural bases for constructing quantum two level systems, or qubits, in semiconductor quantum dots. The quantum dot charge qubit offers a simple architecture and high-speed operation, but generally suffers from fast dephasing due to strong coupling of the environment to the electron's charge. On the other hand, quantum dot spin qubits have demonstrated long coherence times, but their manipulation is often slower than desired for important future applications. This talk will present experimental progress of a `hybrid' qubit, formed by three electrons in a Si/SiGe double quantum dot, which combines desirable characteristics (speed and coherence) in the past found separately in qubits based on either charge or spin degrees of freedom. Using resonant microwaves, we first discuss qubit operations near the `sweet spot' for charge qubit operation. Along with fast (>GHz) manipulation rates for any rotation axis on the Bloch sphere, we implement two independent tomographic characterization schemes in the charge qubit regime: traditional quantum process tomography (QPT) and gate set tomography (GST). We also present resonant qubit operations of the hybrid qubit performed on the same device, DC pulsed gate operations of which were recently demonstrated. We demonstrate three-axis control and the implementation of dynamic decoupling pulse sequences. Performing QPT on the hybrid qubit, we show that AC gating yields π rotation process fidelities higher than 93% for X-axis and 96% for Z-axis rotations, which demonstrates efficient quantum control of semiconductor qubits using resonant microwaves. We discuss a path forward for achieving fidelities better than the threshold for quantum error correction using surface codes. This work was supported in part by ARO (W911NF-12-0607), NSF (PHY-1104660), DOE (DE-FG02-03ER46028), and by the Laboratory Directed Research and Development program at Sandia National Laboratories
Theory of the Quantum Dot Hybrid Qubit
Friesen, Mark
2015-03-01
The quantum dot hybrid qubit, formed from three electrons in two quantum dots, combines the desirable features of charge qubits (fast manipulation) and spin qubits (long coherence times). The hybridized spin and charge states yield a unique energy spectrum with several useful properties, including two different operating regimes that are relatively immune to charge noise due to the presence of optimal working points or ``sweet spots.'' In this talk, I will describe dc and ac-driven gate operations of the quantum dot hybrid qubit. I will analyze improvements in the dephasing that are enabled by the sweet spots, and I will discuss the outlook for quantum hybrid qubits in terms of scalability. This work was supported in part by ARO (W911NF-12-0607), NSF (PHY-1104660), the USDOD, and the Intelligence Community Postdoctoral Research Fellowship Program. The views and conclusions contained in this presentation are those of the authors and should not be interpreted as representing the official policies or endorsements, either expressed or implied, of the US government.
Hybrid quantum teleportation: A theoretical model
Energy Technology Data Exchange (ETDEWEB)
Takeda, Shuntaro; Mizuta, Takahiro; Fuwa, Maria; Yoshikawa, Jun-ichi; Yonezawa, Hidehiro; Furusawa, Akira [Department of Applied Physics, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656 (Japan)
2014-12-04
Hybrid quantum teleportation – continuous-variable teleportation of qubits – is a promising approach for deterministically teleporting photonic qubits. We propose how to implement it with current technology. Our theoretical model shows that faithful qubit transfer can be achieved for this teleportation by choosing an optimal gain for the teleporter’s classical channel.
Ferenczy, György G
2013-04-05
Mixed quantum mechanics/quantum mechanics (QM/QM) and quantum mechanics/molecular mechanics (QM/MM) methods make computations feasible for extended chemical systems by separating them into subsystems that are treated at different level of sophistication. In many applications, the subsystems are covalently bound and the use of frozen localized orbitals at the boundary is a possible way to separate the subsystems and to ensure a sensible description of the electronic structure near to the boundary. A complication in these methods is that orthogonality between optimized and frozen orbitals has to be warranted and this is usually achieved by an explicit orthogonalization of the basis set to the frozen orbitals. An alternative to this approach is proposed by calculating the wave-function from the Huzinaga equation that guaranties orthogonality to the frozen orbitals without basis set orthogonalization. The theoretical background and the practical aspects of the application of the Huzinaga equation in mixed methods are discussed. Forces have been derived to perform geometry optimization with wave-functions from the Huzinaga equation. Various properties have been calculated by applying the Huzinaga equation for the central QM subsystem, representing the environment by point charges and using frozen strictly localized orbitals to connect the subsystems. It is shown that a two to three bond separation of the chemical or physical event from the frozen bonds allows a very good reproduction (typically around 1 kcal/mol) of standard Hartree-Fock-Roothaan results. The proposed scheme provides an appropriate framework for mixed QM/QM and QM/MM methods. Copyright © 2012 Wiley Periodicals, Inc.
Bueren-Calabuig, Juan A; Pierdominici-Sottile, Gustavo; Roitberg, Adrian E
2014-06-05
Chagas' disease, also known as American trypanosomiasis, is a lethal, chronic disease that currently affects more than 10 million people in Central and South America. The trans-sialidase from Trypanosoma cruzi (T. cruzi, TcTS) is a crucial enzyme for the survival of this parasite: sialic acids from the host are transferred to the cell surface glycoproteins of the trypanosome, thereby evading the host's immune system. On the other hand, the sialidase of T. rangeli (TrSA), which shares 70% sequence identity with TcTS, is a strict hydrolase and shows no trans-sialidase activity. Therefore, TcTS and TrSA represent an excellent framework to understand how different catalytic activities can be achieved with extremely similar structures. By means of combined quantum mechanics-molecular mechanics (QM/MM, SCC-DFTB/Amberff99SB) calculations and umbrella sampling simulations, we investigated the hydrolysis mechanisms of TcTS and TrSA and computed the free energy profiles of these reactions. The results, together with our previous computational investigations, are able to explain the catalytic mechanism of sialidases and describe how subtle differences in the active site make TrSA a strict hydrolase and TcTS a more efficient trans-sialidase.
Woods, Christopher J; Shaw, Katherine E; Mulholland, Adrian J
2015-01-22
The applicability of combined quantum mechanics/molecular mechanics (QM/MM) methods for the calculation of absolute binding free energies of conserved water molecules in protein/ligand complexes is demonstrated. Here, we apply QM/MM Monte Carlo simulations to investigate binding of water molecules to influenza neuraminidase. We investigate five different complexes, including those with the drugs oseltamivir and peramivir. We investigate water molecules in two different environments, one more hydrophobic and one hydrophilic. We calculate the free-energy change for perturbation of a QM to MM representation of the bound water molecule. The calculations are performed at the BLYP/aVDZ (QM) and TIP4P (MM) levels of theory, which we have previously demonstrated to be consistent with one another for QM/MM modeling. The results show that the QM to MM perturbation is significant in both environments (greater than 1 kcal mol(-1)) and larger in the more hydrophilic site. Comparison with the same perturbation in bulk water shows that this makes a contribution to binding. The results quantify how electronic polarization differences in different environments affect binding affinity and also demonstrate that extensive, converged QM/MM free-energy simulations, with good levels of QM theory, are now practical for protein/ligand complexes.
Pang, Jiayun; Scrutton, Nigel S; Sutcliffe, Michael J
2014-09-01
A computational study was performed on the experimentally elusive cyclisation step in the cofactor pyridoxal 5'-phosphate (PLP)-dependent D-ornithine 4,5-aminomutase (OAM)-catalysed reaction. Calculations using both model systems and a combined quantum mechanics/molecular mechanics approach suggest that regulation of the cyclic radical intermediate is achieved through the synergy of the intrinsic catalytic power of cofactor PLP and the active site of the enzyme. The captodative effect of PLP is balanced by an enzyme active site that controls the deprotonation of both the pyridine nitrogen atom (N1) and the Schiff-base nitrogen atom (N2). Furthermore, electrostatic interactions between the terminal carboxylate and amino groups of the substrate and Arg297 and Glu81 impose substantial "strain" energy on the orientation of the cyclic intermediate to control its trajectory. In addition the "strain" energy, which appears to be sensitive to both the number of carbon atoms in the substrate/analogue and the position of the radical intermediates, may play a key role in controlling the transition of the enzyme from the closed to the open state. Our results provide new insights into several aspects of the radical mechanism in aminomutase catalysis and broaden our understanding of cofactor PLP-dependent reactions. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Wang, Jimin; Askerka, Mikhail; Brudvig, Gary W; Batista, Victor S
2017-02-10
Understanding structure-function relations in photosystem II (PSII) is important for the development of biomimetic photocatalytic systems. X-ray crystallography, computational modeling, and spectroscopy have played central roles in elucidating the structure and function of PSII. Recent breakthroughs in femtosecond X-ray crystallography offer the possibility of collecting diffraction data from the X-ray free electron laser (XFEL) before radiation damage of the sample, thereby overcoming the main challenge of conventional X-ray diffraction methods. However, the interpretation of XFEL data from PSII intermediates is challenging because of the issues regarding data-processing, uncertainty on the precise positions of light oxygen atoms next to heavy metal centers, and different kinetics of the S-state transition in microcrystals compared to solution. Here, we summarize recent advances and outstanding challenges in PSII structure-function determination with emphasis on the implementation of quantum mechanics/molecular mechanics techniques combined with isomorphous difference Fourier maps, direct methods, and high-resolution spectroscopy.
Nakamura, Shin; Noguchi, Takumi
2016-10-11
During photosynthesis, the light-driven oxidation of water performed by photosystem II (PSII) provides electrons necessary to fix CO 2 , in turn supporting life on Earth by liberating molecular oxygen. Recent high-resolution X-ray images of PSII show that the water-oxidizing center (WOC) is composed of an Mn 4 CaO 5 cluster with six carboxylate, one imidazole, and four water ligands. FTIR difference spectroscopy has shown significant structural changes of the WOC during the S-state cycle of water oxidation, especially within carboxylate groups. However, the roles that these carboxylate groups play in water oxidation as well as how they should be properly assigned in spectra are unresolved. In this study, we performed a normal mode analysis of the WOC using the quantum mechanics/molecular mechanics (QM/MM) method to simulate FTIR difference spectra on the S 1 to S 2 transition in the carboxylate stretching region. By evaluating WOC models with different oxidation and protonation states, we determined that models of high-oxidation states, Mn(III) 2 Mn(IV) 2 , satisfactorily reproduced experimental spectra from intact and Ca-depleted PSII compared with low-oxidation models. It is further suggested that the carboxylate groups bridging Ca and Mn ions within this center tune the reactivity of water ligands bound to Ca by shifting charge via their π conjugation.
Raich, Lluís; Borodkin, Vladimir; Fang, Wenxia; Castro-López, Jorge; van Aalten, Daan M F; Hurtado-Guerrero, Ramón; Rovira, Carme
2016-03-16
The conversion of glycoside hydrolases (GHs) into transglycosylases (TGs), i.e., from enzymes that hydrolyze carbohydrates to enzymes that synthesize them, represents a promising solution for the large-scale synthesis of complex carbohydrates for biotechnological purposes. However, the lack of knowledge about the molecular details of transglycosylation hampers the rational design of TGs. Here we present the first crystallographic structure of a natural glycosyl-enzyme intermediate (GEI) of Saccharomyces cerevisiae Gas2 in complex with an acceptor substrate and demonstrate, by means of quantum mechanics/molecular mechanics metadynamics simulations, that it is tuned for transglycosylation (ΔG(⧧) = 12 kcal/mol). The 2-OH···nucleophile interaction is found to be essential for catalysis: its removal raises the free energy barrier significantly (11 and 16 kcal/mol for glycosylation and transglycosylation, respectively) and alters the conformational itinerary of the substrate (from (4)C1 → [(4)E](⧧) → (1,4)B/(4)E to (4)C1 → [(4)H3](⧧) → (4)C1). Our results suggest that changes in the interactions involving the 2-position could have an impact on the transglycosylation activity of several GHs.
Dohn, A O; Jónsson, E Ö; Levi, G; Mortensen, J J; Lopez-Acevedo, O; Thygesen, K S; Jacobsen, K W; Ulstrup, J; Henriksen, N E; Møller, K B; Jónsson, H
2017-12-12
A multiscale density functional theory-quantum mechanics/molecular mechanics (DFT-QM/MM) scheme is presented, based on an efficient electrostatic coupling between the electronic density obtained from a grid-based projector augmented wave (GPAW) implementation of density functional theory and a classical potential energy function. The scheme is implemented in a general fashion and can be used with various choices for the descriptions of the QM or MM regions. Tests on H 2 O clusters, ranging from dimer to decamer show that no systematic energy errors are introduced by the coupling that exceeds the differences in the QM and MM descriptions. Over 1 ns of liquid water, Born-Oppenheimer QM/MM molecular dynamics (MD) are sampled combining 10 parallel simulations, showing consistent liquid water structure over the QM/MM border. The method is applied in extensive parallel MD simulations of an aqueous solution of the diplatinum [Pt 2 (P 2 O 5 H 2 ) 4 ] 4- complex (PtPOP), spanning a total time period of roughly half a nanosecond. An average Pt-Pt distance deviating only 0.01 Å from experimental results, and a ground-state Pt-Pt oscillation frequency deviating by <2% from experimental results were obtained. The simulations highlight a remarkable harmonicity of the Pt-Pt oscillation, while also showing clear signs of Pt-H hydrogen bonding and directional coordination of water molecules along the Pt-Pt axis of the complex.
Quesne, Matthew G; Latifi, Reza; Gonzalez-Ovalle, Luis E; Kumar, Devesh; de Visser, Sam P
2014-01-01
AlkB repair enzymes are important nonheme iron enzymes that catalyse the demethylation of alkylated DNA bases in humans, which is a vital reaction in the body that heals externally damaged DNA bases. Its mechanism is currently controversial and in order to resolve the catalytic mechanism of these enzymes, a quantum mechanics/molecular mechanics (QM/MM) study was performed on the demethylation of the N1-methyladenine fragment by AlkB repair enzymes. Firstly, the initial modelling identified the oxygen binding site of the enzyme. Secondly, the oxygen activation mechanism was investigated and a novel pathway was found, whereby the catalytically active iron(IV)–oxo intermediate in the catalytic cycle undergoes an initial isomerisation assisted by an Arg residue in the substrate binding pocket, which then brings the oxo group in close contact with the methyl group of the alkylated DNA base. This enables a subsequent rate-determining hydrogen-atom abstraction on competitive σ-and π-pathways on a quintet spin-state surface. These findings give evidence of different locations of the oxygen and substrate binding channels in the enzyme and the origin of the separation of the oxygen-bound intermediates in the catalytic cycle from substrate. Our studies are compared with small model complexes and the effect of protein and environment on the kinetics and mechanism is explained. PMID:24339041
Energy Technology Data Exchange (ETDEWEB)
Ngaojampa, C.; Nimmanpipug, P. [Computer Simulation and Modeling Laboratory (CSML), Department of Chemistry and Center for Innovation Chemistry, Faculty of Science, Chiang Mai University, Chiang Mai 50200 (Thailand); Yu, L.D., E-mail: yuld@fnrf.science.cmu.ac.t [Plasma and Beam Physics Research Facility, Department of Physics and Materials Science, Faculty of Science, Chiang Mai University, Chiang Mai 50200 (Thailand); Thailand Center of Excellence in Physics, Commission on Higher Education, 328 Si Ayutthaya Road, Bangkok 10400 (Thailand); Anuntalabhochai, S. [Molecular Biology Laboratory, Department of Biology, Faculty of Science, Chiang Mai University, Chiang Mai 50200 (Thailand); Lee, V.S., E-mail: vannajan@gmail.co [Computer Simulation and Modeling Laboratory (CSML), Department of Chemistry and Center for Innovation Chemistry, Faculty of Science, Chiang Mai University, Chiang Mai 50200 (Thailand); Thailand Center of Excellence in Physics, Commission on Higher Education, 328 Si Ayutthaya Road, Bangkok 10400 (Thailand)
2011-02-15
In order to promote understanding of the fundamentals of ultra-low-energy ion interaction with DNA, molecular dynamics simulations using combined quantum-mechanics/molecular-mechanics of poly-AT and poly-GC A-DNA double strands irradiated by <200 eV carbon ions were performed to investigate the molecular implications of mutation bias. The simulations were focused on the responses of the DNA backbones and nitrogenous bases to irradiation. Analyses of the root mean square displacements of the backbones and non-hydrogen atoms of base rings of the simulated DNA structure after irradiation revealed a potential preference of DNA double strand separation, dependent on the irradiating energy. The results show that for the backbones, the large difference in the displacement between poly-GC and poly-AT in the initial time period could be the reason for the backbone breakage; for the nitrogenous base pairs, A-T is 30% more sensitive or vulnerable to ion irradiation than G-C, demonstrating a preferential, instead of random, effect of irradiation-induced mutation.
International Nuclear Information System (INIS)
Ngaojampa, C.; Nimmanpipug, P.; Yu, L.D.; Anuntalabhochai, S.; Lee, V.S.
2011-01-01
In order to promote understanding of the fundamentals of ultra-low-energy ion interaction with DNA, molecular dynamics simulations using combined quantum-mechanics/molecular-mechanics of poly-AT and poly-GC A-DNA double strands irradiated by <200 eV carbon ions were performed to investigate the molecular implications of mutation bias. The simulations were focused on the responses of the DNA backbones and nitrogenous bases to irradiation. Analyses of the root mean square displacements of the backbones and non-hydrogen atoms of base rings of the simulated DNA structure after irradiation revealed a potential preference of DNA double strand separation, dependent on the irradiating energy. The results show that for the backbones, the large difference in the displacement between poly-GC and poly-AT in the initial time period could be the reason for the backbone breakage; for the nitrogenous base pairs, A-T is 30% more sensitive or vulnerable to ion irradiation than G-C, demonstrating a preferential, instead of random, effect of irradiation-induced mutation.
Uchida, Satoshi; Yoshida, Taketo; Tochikubo, Fumiyoshi
2017-10-01
Plasma medicine is one of the most attractive applications using atmospheric pressure nonequilibrium plasma. With respect to direct contact of the discharge plasma with a biological membrane, reactive oxygen species play an important role in induction of medical effects. However, complicated interactions between the plasma radicals and membrane have not been understood well. In the present work, we simulated elemental processes at the first stage of physicochemical interactions between oxygen atom and phosphatidylcholine using the quantum mechanical molecular dynamics code in a general software AMBER. The change in the above processes was classified according to the incident energy of oxygen atom. At an energy of 1 eV, the abstraction of a hydrogen atom and recombination to phosphatidylcholine were simultaneously occurred in chemical attachment of incident oxygen atom. The exothermal energy of the reaction was about 80% of estimated one based on the bond energies of ethane. An oxygen atom over 10 eV separated phosphatidylcholine partially. The behaviour became increasingly similar to physical sputtering. The reaction probability of oxygen atom was remarkably high in comparison with that of hydrogen peroxide. These results suggest that we can uniformly estimate various physicochemical dynamics of reactive oxygen species against membrane lipids.
Dong, Minghui; Liu, Haiyan
2008-08-21
The Escherichia coli peptide deformylase (PDF) and Bacillus thermoproteolyticus thermolysin (TLN) are two representative metal-requiring peptidases having remarkably similar active centers but distinctively different metal preferences. Zinc is a competent catalytic cofactor for TLN but not for PDF. Reaction pathways and the associated energetics for both enzymes were determined using combined semiempirical and ab initio quantum mechanical/molecular mechanical modeling, without presuming reaction coordinates. The results confirmed that both enzymes catalyze via the same chemical steps, and reproduced their different preferences for zinc or iron as competent cofactors. Further analyses indicated that different feasibility of the nucleophilic attack step leads to different metal preferences of the two enzymes. In TLN, the substrate is strongly activated and can serve as the fifth coordination ligand of zinc prior to the chemical steps. In PDF, the substrate carbonyl is activated by the chemical step itself, and becomes the fifth coordination partner of zinc only in a later stage of the nucleophilic attack. These leads to a much more difficult nucleophilic attack in PDF than in TLN. Different from some earlier suggestions, zinc has no difficulty in accepting an activated substrate as the fifth ligand to switch from tetra- to penta-coordination in either PDF or TLN. When iron replaces zinc, its stronger interaction with the hydroxide ligand may lead to higher activation barrier in TLN. In PDF, the stronger interactions of iron with ligands allow iron-substrate coordination to take place either before or at a very early stage of the chemical step, leading to effective catalysis. Our calculations also show combined semiempirical and ab initio quantum mechanical modeling can be efficient approaches to explore complicated reaction pathways in enzyme systems.
Develop of a quantum electromechanical hybrid system
Hao, Yu; Rouxinol, Francisco; Brito, Frederico; Caldeira, Amir; Irish, Elinor; Lahaye, Matthew
In this poster, we will show our results from measurements of a hybrid quantum system composed of a superconducting transmon qubit-coupled and ultra-high frequency nano-mechanical resonator, embedded in a superconducting cavity. The transmon is capacitively coupled to a 3.4GHz nanoresonator and a T-filter-biased high-Q transmission line cavity. Single-tone and two-tone transmission spectroscopy measurements are used to probe the interactions between the cavity, qubit and mechanical resonator. These measurements are in good agreement with numerical simulations based upon a master equation for the tripartite system including dissipation. The results indicate that this system may be developed to serve as a platform for more advanced measurements with nanoresonators, including quantum state measurement, the exploration of nanoresonator quantum noise, and reservoir engineering.
Monari, Antonio; Rivail, Jean-Louis; Assfeld, Xavier
2013-02-19
Molecular mechanics methods can efficiently compute the macroscopic properties of a large molecular system but cannot represent the electronic changes that occur during a chemical reaction or an electronic transition. Quantum mechanical methods can accurately simulate these processes, but they require considerably greater computational resources. Because electronic changes typically occur in a limited part of the system, such as the solute in a molecular solution or the substrate within the active site of enzymatic reactions, researchers can limit the quantum computation to this part of the system. Researchers take into account the influence of the surroundings by embedding this quantum computation into a calculation of the whole system described at the molecular mechanical level, a strategy known as the mixed quantum mechanics/molecular mechanics (QM/MM) approach. The accuracy of this embedding varies according to the types of interactions included, whether they are purely mechanical or classically electrostatic. This embedding can also introduce the induced polarization of the surroundings. The difficulty in QM/MM calculations comes from the splitting of the system into two parts, which requires severing the chemical bonds that link the quantum mechanical subsystem to the classical subsystem. Typically, researchers replace the quantoclassical atoms, those at the boundary between the subsystems, with a monovalent link atom. For example, researchers might add a hydrogen atom when a C-C bond is cut. This Account describes another approach, the Local Self Consistent Field (LSCF), which was developed in our laboratory. LSCF links the quantum mechanical portion of the molecule to the classical portion using a strictly localized bond orbital extracted from a small model molecule for each bond. In this scenario, the quantoclassical atom has an apparent nuclear charge of +1. To achieve correct bond lengths and force constants, we must take into account the inner shell of
Pitari, Fabio; Bovi, Daniele; Narzi, Daniele; Guidoni, Leonardo
2015-09-29
The Mn4CaO5 cluster in the oxygen-evolving complex is the catalytic core of the Photosystem II (PSII) enzyme, responsible for the water splitting reaction in oxygenic photosynthesis. The role of the redox-inactive ion in the cluster has not yet been fully clarified, although several experimental data are available on Ca2+-depleted and Ca2+-substituted PSII complexes, indicating Sr2+-substituted PSII as the only modification that preserves oxygen evolution. In this work, we investigated the structural and electronic properties of the PSII catalytic core with Ca2+ replaced with Sr2+ and Cd2+ in the S2 state of the Kok−Joliot cycle by means of density functional theory and ab initio molecular dynamics based on a quantum mechanics/ molecular mechanics approach. Our calculations do not reveal significant differences between the substituted and wild-type systems in terms of geometries, thermodynamics, and kinetics of two previously identified intermediate states along the S2 to S3 transition, namely, the open cubane S2 A and closed cubane S2 B conformers. Conversely, our calculations show different pKa values for the water molecule bound to the three investigated heterocations. Specifically, for Cd-substituted PSII, the pKa value is 5.3 units smaller than the respective value in wild type Ca-PSII. On the basis of our results, we conclude that, assuming all the cations sharing the same binding site, the induced difference in the acidity of the binding pocket might influence the hydrogen bonding network and the redox levels to prevent the further evolution of the cycle toward the S3 state.
Song, Xudan; Lu, Jiarui; Lai, Wenzhen
2017-08-02
Herein, we use in-protein quantum mechanical/molecular mechanical (QM/MM) calculations to elucidate the mechanism of dioxygen activation, oxygen atom exchange and substrate epoxidation processes by AsqJ, an Fe II /α-ketoglutarate-dependent dioxygenase (α-KGD) using a 2-His-1-Asp facial triad. Our results demonstrated that the whole reaction proceeds through a quintet surface. The dioxygen activation by AsqJ leads to a quintet penta-coordinated Fe IV -oxo species, which has a square pyramidal geometry with the oxo group trans to His134. This penta-coordinated Fe IV -oxo species is not the reactive one in the substrate epoxidation reaction since its oxo group is pointing away from the target C[double bond, length as m-dash]C bond. Instead, it can undergo the oxo group isomerization followed by water binding or the water binding followed by oxygen atom exchange to form the reactive hexa-coordinated Fe IV -oxo species with the oxo group trans to His211. The calculated parameters of Mössbauer spectra for this hexa-coordinated Fe IV -oxo intermediate are in excellent agreement with the experimental values, suggesting that it is most likely the experimentally trapped species. The calculated energetics indicated that the rate-limiting step is the substrate C[double bond, length as m-dash]C bond activation. This work improves our understanding of the dioxygen activation by α-KGD and provides important structural information about the reactive Fe IV -oxo species.
Hybrid passivated colloidal quantum dot solids
Ip, Alex
2012-07-29
Colloidal quantum dot (CQD) films allow large-area solution processing and bandgap tuning through the quantum size effect. However, the high ratio of surface area to volume makes CQD films prone to high trap state densities if surfaces are imperfectly passivated, promoting recombination of charge carriers that is detrimental to device performance. Recent advances have replaced the long insulating ligands that enable colloidal stability following synthesis with shorter organic linkers or halide anions, leading to improved passivation and higher packing densities. Although this substitution has been performed using solid-state ligand exchange, a solution-based approach is preferable because it enables increased control over the balance of charges on the surface of the quantum dot, which is essential for eliminating midgap trap states. Furthermore, the solution-based approach leverages recent progress in metal:chalcogen chemistry in the liquid phase. Here, we quantify the density of midgap trap states in CQD solids and show that the performance of CQD-based photovoltaics is now limited by electrong-"hole recombination due to these states. Next, using density functional theory and optoelectronic device modelling, we show that to improve this performance it is essential to bind a suitable ligand to each potential trap site on the surface of the quantum dot. We then develop a robust hybrid passivation scheme that involves introducing halide anions during the end stages of the synthesis process, which can passivate trap sites that are inaccessible to much larger organic ligands. An organic crosslinking strategy is then used to form the film. Finally, we use our hybrid passivated CQD solid to fabricate a solar cell with a certified efficiency of 7.0%, which is a record for a CQD photovoltaic device. © 2012 Macmillan Publishers Limited. All rights reserved.
Hybrid passivated colloidal quantum dot solids
Ip, Alex; Thon, Susanna; Hoogland, Sjoerd H.; Voznyy, Oleksandr; Zhitomirsky, David; Debnath, Ratan K.; Levina, Larissa; Rollny, Lisa R.; Carey, Graham H.; Fischer, Armin H.; Kemp, Kyle W.; Kramer, Illan J.; Ning, Zhijun; Labelle, André J.; Chou, Kang Wei; Amassian, Aram; Sargent, E. H.
2012-01-01
Colloidal quantum dot (CQD) films allow large-area solution processing and bandgap tuning through the quantum size effect. However, the high ratio of surface area to volume makes CQD films prone to high trap state densities if surfaces are imperfectly passivated, promoting recombination of charge carriers that is detrimental to device performance. Recent advances have replaced the long insulating ligands that enable colloidal stability following synthesis with shorter organic linkers or halide anions, leading to improved passivation and higher packing densities. Although this substitution has been performed using solid-state ligand exchange, a solution-based approach is preferable because it enables increased control over the balance of charges on the surface of the quantum dot, which is essential for eliminating midgap trap states. Furthermore, the solution-based approach leverages recent progress in metal:chalcogen chemistry in the liquid phase. Here, we quantify the density of midgap trap states in CQD solids and show that the performance of CQD-based photovoltaics is now limited by electrong-"hole recombination due to these states. Next, using density functional theory and optoelectronic device modelling, we show that to improve this performance it is essential to bind a suitable ligand to each potential trap site on the surface of the quantum dot. We then develop a robust hybrid passivation scheme that involves introducing halide anions during the end stages of the synthesis process, which can passivate trap sites that are inaccessible to much larger organic ligands. An organic crosslinking strategy is then used to form the film. Finally, we use our hybrid passivated CQD solid to fabricate a solar cell with a certified efficiency of 7.0%, which is a record for a CQD photovoltaic device. © 2012 Macmillan Publishers Limited. All rights reserved.
Wang, Binju; Li, Chunsen; Dubey, Kshatresh Dutta; Shaik, Sason
2015-06-17
Quantum mechanical/molecular mechanical calculations address the longstanding-question of a "second oxidant" in P450 enzymes wherein the proton-shuttle, which leads to formation of the "primary-oxidant" Compound I (Cpd I), was severed by mutating the crucial residue (in P450cam: Threonine-252-to-Alanine, hence T252A). Investigating the oxidant candidates Cpd I, ferric hydroperoxide, and ferric hydrogen peroxide (Fe(III)(O2H2)), and their reactions, generates reactivity networks which enable us to rule out a "second oxidant" and at the same time identify an additional coupling pathway that is responsible for the epoxidation of 5-methylenylcamphor by the T252A mutant. In this "second-coupling pathway", the reaction starts with the Fe(III)(O2H2) intermediate, which transforms to Cpd I via a O-O homolysis/H-abstraction mechanism. The persistence of Fe(III)(O2H2) and its oxidative reactivity are shown to be determined by interplay of substrate and protein. The substrate 5-methylenylcamphor prevents H2O2 release, while the protein controls the Fe(III)(O2H2) conversion to Cpd I by nailing-through hydrogen-bonding interactions-the conformation of the HO(•) radical produced during O-O homolysis. This conformation prevents HO(•) attack on the porphyrin's meso position, as in heme oxygenase, and prefers H-abstraction from Fe(IV)OH thereby generating H2O + Cpd I. Cpd I then performs substrate oxidations. Camphor cannot prevent H2O2 release and hence the T252A mutant does not oxidize camphor. This "second pathway" transpires also during H2O2 shunting of the cycle of wild-type P450cam, where the additional hydrogen-bonding with Thr252 prevents H2O2 release, and contributes to a successful Cpd I formation. The present results lead to a revised catalytic cycle of Cytochrome P450cam.
Quantum-classical hybrid dynamics – a summary
International Nuclear Information System (INIS)
Elze, Hans-Thomas
2013-01-01
A summary of a recently proposed description of quantum-classical hybrids is presented, which concerns quantum and classical degrees of freedom of a composite object that interact directly with each other. This is based on notions of classical Hamiltonian mechanics suitably extended to quantum mechanics.
Adaptive hybrid optimal quantum control for imprecisely characterized systems.
Egger, D J; Wilhelm, F K
2014-06-20
Optimal quantum control theory carries a huge promise for quantum technology. Its experimental application, however, is often hindered by imprecise knowledge of the input variables, the quantum system's parameters. We show how to overcome this by adaptive hybrid optimal control, using a protocol named Ad-HOC. This protocol combines open- and closed-loop optimal control by first performing a gradient search towards a near-optimal control pulse and then an experimental fidelity estimation with a gradient-free method. For typical settings in solid-state quantum information processing, adaptive hybrid optimal control enhances gate fidelities by an order of magnitude, making optimal control theory applicable and useful.
Quantum-Classical Hybrid for Information Processing
Zak, Michail
2011-01-01
Based upon quantum-inspired entanglement in quantum-classical hybrids, a simple algorithm for instantaneous transmissions of non-intentional messages (chosen at random) to remote distances is proposed. The idea is to implement instantaneous transmission of conditional information on remote distances via a quantum-classical hybrid that preserves superposition of random solutions, while allowing one to measure its state variables using classical methods. Such a hybrid system reinforces the advantages, and minimizes the limitations, of both quantum and classical characteristics. Consider n observers, and assume that each of them gets a copy of the system and runs it separately. Although they run identical systems, the outcomes of even synchronized runs may be different because the solutions of these systems are random. However, the global constrain must be satisfied. Therefore, if the observer #1 (the sender) made a measurement of the acceleration v(sub 1) at t =T, then the receiver, by measuring the corresponding acceleration v(sub 1) at t =T, may get a wrong value because the accelerations are random, and only their ratios are deterministic. Obviously, the transmission of this knowledge is instantaneous as soon as the measurements have been performed. In addition to that, the distance between the observers is irrelevant because the x-coordinate does not enter the governing equations. However, the Shannon information transmitted is zero. None of the senders can control the outcomes of their measurements because they are random. The senders cannot transmit intentional messages. Nevertheless, based on the transmitted knowledge, they can coordinate their actions based on conditional information. If the observer #1 knows his own measurements, the measurements of the others can be fully determined. It is important to emphasize that the origin of entanglement of all the observers is the joint probability density that couples their actions. There is no centralized source
Hydrogen atom as a quantum-classical hybrid system
International Nuclear Information System (INIS)
Zhan, Fei; Wu, Biao
2013-01-01
Hydrogen atom is studied as a quantum-classical hybrid system, where the proton is treated as a classical object while the electron is regarded as a quantum object. We use a well known mean-field approach to describe this hybrid hydrogen atom; the resulting dynamics for the electron and the proton is compared to their full quantum dynamics. The electron dynamics in the hybrid description is found to be only marginally different from its full quantum counterpart. The situation is very different for the proton: in the hybrid description, the proton behaves like a free particle; in the fully quantum description, the wave packet center of the proton orbits around the center of mass. Furthermore, we find that the failure to describe the proton dynamics properly can be regarded as a manifestation of the fact that there is no conservation of momentum in the mean-field hybrid approach. We expect that such a failure is a common feature for all existing approaches for quantum-classical hybrid systems of Born-Oppenheimer type.
Hybrid cluster state proposal for a quantum game
International Nuclear Information System (INIS)
Paternostro, M; Tame, M S; Kim, M S
2005-01-01
We propose an experimental implementation of a quantum game algorithm in a hybrid scheme combining the quantum circuit approach and the cluster state model. An economical cluster configuration is suggested to embody a quantum version of the Prisoners' Dilemma. Our proposal is shown to be within the experimental state of the art and can be realized with existing technology.The effects of relevant experimental imperfections are also carefully examined
Fano Effect and Quantum Entanglement in Hybrid Semiconductor Quantum Dot-Metal Nanoparticle System.
He, Yong; Zhu, Ka-Di
2017-06-20
In this paper, we review the investigation for the light-matter interaction between surface plasmon field in metal nanoparticle (MNP) and the excitons in semiconductor quantum dots (SQDs) in hybrid SQD-MNP system under the full quantum description. The exciton-plasmon interaction gives rise to the modified decay rate and the exciton energy shift which are related to the exciton energy by using a quantum transformation method. We illustrate the responses of the hybrid SQD-MNP system to external field, and reveal Fano effect shown in the absorption spectrum. We demonstrate quantum entanglement between two SQD mediated by surface plasmon field. In the absence of a laser field, concurrence of quantum entanglement will disappear after a few ns. If the laser field is present, the steady states appear, so that quantum entanglement produced will reach a steady-state entanglement. Because one of all optical pathways to induce Fano effect refers to the generation of quantum entangled states, It is shown that the concurrence of quantum entanglement can be obtained by observation for Fano effect. In a hybrid system including two MNP and a SQD, because the two Fano quantum interference processes share a segment of all optical pathways, there is correlation between the Fano effects of the two MNP. The investigations for the light-matter interaction in hybrid SQD-MNP system can pave the way for the development of the optical processing devices and quantum information based on the exciton-plasmon interaction.
Fano Effect and Quantum Entanglement in Hybrid Semiconductor Quantum Dot-Metal Nanoparticle System
Directory of Open Access Journals (Sweden)
Yong He
2017-06-01
Full Text Available In this paper, we review the investigation for the light-matter interaction between surface plasmon field in metal nanoparticle (MNP and the excitons in semiconductor quantum dots (SQDs in hybrid SQD-MNP system under the full quantum description. The exciton-plasmon interaction gives rise to the modified decay rate and the exciton energy shift which are related to the exciton energy by using a quantum transformation method. We illustrate the responses of the hybrid SQD-MNP system to external field, and reveal Fano effect shown in the absorption spectrum. We demonstrate quantum entanglement between two SQD mediated by surface plasmon field. In the absence of a laser field, concurrence of quantum entanglement will disappear after a few ns. If the laser field is present, the steady states appear, so that quantum entanglement produced will reach a steady-state entanglement. Because one of all optical pathways to induce Fano effect refers to the generation of quantum entangled states, It is shown that the concurrence of quantum entanglement can be obtained by observation for Fano effect. In a hybrid system including two MNP and a SQD, because the two Fano quantum interference processes share a segment of all optical pathways, there is correlation between the Fano effects of the two MNP. The investigations for the light-matter interaction in hybrid SQD-MNP system can pave the way for the development of the optical processing devices and quantum information based on the exciton-plasmon interaction.
International Nuclear Information System (INIS)
Pei Pei; He-Fei Huang; Yan-Qing Guo; He-Shan Song
2016-01-01
We develop a design of a hybrid quantum interface for quantum information transfer (QIT), adopting a nanomechanical resonator as the intermedium, which is magnetically coupled with individual nitrogen-vacancy centers as the solid qubits, while capacitively coupled with a coplanar waveguide resonator as the quantum data bus. We describe the Hamiltonian of the model, and analytically demonstrate the QIT for both the resonant interaction and large detuning cases. The hybrid quantum interface allows for QIT between arbitrarily selected individual nitrogen-vacancy centers, and has advantages of the scalability and controllability. Our methods open an alternative perspective for implementing QIT, which is important during quantum storing or processing procedures in quantum computing. (paper)
Tunable Hybrid Qubit in a Triple Quantum Dot
Wang, Bao-Chuan; Cao, Gang; Li, Hai-Ou; Xiao, Ming; Guo, Guang-Can; Hu, Xuedong; Jiang, Hong-Wen; Guo, Guo-Ping
2017-12-01
We experimentally demonstrate quantum-coherent dynamics of a triple-dot-based multielectron hybrid qubit. Pulsed experiments show that this system can be conveniently initialized, controlled, measured electrically, and has a good ratio Q ˜29 between the coherence time and gate time. Furthermore, the current multielectron hybrid qubit has an operation frequency that is tunable in a wide range, from 2 to about 15 GHz. We also provide a qualitative understanding of the experimental observations by mapping them onto a three-electron system. The demonstration of the high tunability in a triple dot system could be potentially useful for future quantum control.
Graphene quantum dots-carbon nanotube hybrid arrays for supercapacitors
Hu, Yue; Zhao, Yang; Lu, Gewu; Chen, Nan; Zhang, Zhipan; Li, Hui; Shao, Huibo; Qu, Liangti
2013-05-01
Graphene quantum dots (GQDs) have been successfully deposited onto aligned carbon nanotubes (CNTs) by a benign electrochemical method and the capacitive properties of the as-formed GQD/CNT hybrid arrays were evaluated in symmetrical supercapacitors. It was found that supercapacitors fabricated from GQD/CNT hybrid arrays exhibited a high capacitance of 44 mF cm-2, representing a more than 200% improvement over that of bare CNT electrodes.
Nanogel-quantum dot hybrid nanoparticles for live cell imaging
International Nuclear Information System (INIS)
Hasegawa, Urara; Nomura, Shin-ichiro M.; Kaul, Sunil C.; Hirano, Takashi; Akiyoshi, Kazunari
2005-01-01
We report here a novel carrier of quantum dots (QDs) for intracellular labeling. Monodisperse hybrid nanoparticles (38 nm in diameter) of QDs were prepared by simple mixing with nanogels of cholesterol-bearing pullulan (CHP) modified with amino groups (CHPNH 2 ). The CHPNH 2 -QD nanoparticles were effectively internalized into the various human cells examined. The efficiency of cellular uptake was much higher than that of a conventional carrier, cationic liposome. These hybrid nanoparticles could be a promising fluorescent probe for bioimaging
Nanotetrapods: quantum dot hybrid for bulk heterojunction solar cells
2013-01-01
Hybrid thin film solar cell based on all-inorganic nanoparticles is a new member in the family of photovoltaic devices. In this work, a novel and performance-efficient inorganic hybrid nanostructure with continuous charge transportation and collection channels is demonstrated by introducing CdTe nanotetropods (NTs) and CdSe quantum dots (QDs). Hybrid morphology is characterized, demonstrating an interpenetration and compacted contact of NTs and QDs. Electrical measurements show enhanced charge transfer at the hybrid bulk heterojunction interface of NTs and QDs after ligand exchange which accordingly improves the performance of solar cells. Photovoltaic and light response tests exhibit a combined optic-electric contribution from both CdTe NTs and CdSe QDs through a formation of interpercolation in morphology as well as a type II energy level distribution. The NT and QD hybrid bulk heterojunction is applicable and promising in other highly efficient photovoltaic materials such as PbS QDs. PMID:24139059
Application of fermionic marginal constraints to hybrid quantum algorithms
Rubin, Nicholas C.; Babbush, Ryan; McClean, Jarrod
2018-05-01
Many quantum algorithms, including recently proposed hybrid classical/quantum algorithms, make use of restricted tomography of the quantum state that measures the reduced density matrices, or marginals, of the full state. The most straightforward approach to this algorithmic step estimates each component of the marginal independently without making use of the algebraic and geometric structure of the marginals. Within the field of quantum chemistry, this structure is termed the fermionic n-representability conditions, and is supported by a vast amount of literature on both theoretical and practical results related to their approximations. In this work, we introduce these conditions in the language of quantum computation, and utilize them to develop several techniques to accelerate and improve practical applications for quantum chemistry on quantum computers. As a general result, we demonstrate how these marginals concentrate to diagonal quantities when measured on random quantum states. We also show that one can use fermionic n-representability conditions to reduce the total number of measurements required by more than an order of magnitude for medium sized systems in chemistry. As a practical demonstration, we simulate an efficient restoration of the physicality of energy curves for the dilation of a four qubit diatomic hydrogen system in the presence of three distinct one qubit error channels, providing evidence these techniques are useful for pre-fault tolerant quantum chemistry experiments.
Optimal control of hybrid qubits: Implementing the quantum permutation algorithm
Rivera-Ruiz, C. M.; de Lima, E. F.; Fanchini, F. F.; Lopez-Richard, V.; Castelano, L. K.
2018-03-01
The optimal quantum control theory is employed to determine electric pulses capable of producing quantum gates with a fidelity higher than 0.9997, when noise is not taken into account. Particularly, these quantum gates were chosen to perform the permutation algorithm in hybrid qubits in double quantum dots (DQDs). The permutation algorithm is an oracle based quantum algorithm that solves the problem of the permutation parity faster than a classical algorithm without the necessity of entanglement between particles. The only requirement for achieving the speedup is the use of a one-particle quantum system with at least three levels. The high fidelity found in our results is closely related to the quantum speed limit, which is a measure of how fast a quantum state can be manipulated. Furthermore, we model charge noise by considering an average over the optimal field centered at different values of the reference detuning, which follows a Gaussian distribution. When the Gaussian spread is of the order of 5 μ eV (10% of the correct value), the fidelity is still higher than 0.95. Our scheme also can be used for the practical realization of different quantum algorithms in DQDs.
Coulomb Mediated Hybridization of Excitons in Coupled Quantum Dots.
Ardelt, P-L; Gawarecki, K; Müller, K; Waeber, A M; Bechtold, A; Oberhofer, K; Daniels, J M; Klotz, F; Bichler, M; Kuhn, T; Krenner, H J; Machnikowski, P; Finley, J J
2016-02-19
We report Coulomb mediated hybridization of excitonic states in optically active InGaAs quantum dot molecules. By probing the optical response of an individual quantum dot molecule as a function of the static electric field applied along the molecular axis, we observe unexpected avoided level crossings that do not arise from the dominant single-particle tunnel coupling. We identify a new few-particle coupling mechanism stemming from Coulomb interactions between different neutral exciton states. Such Coulomb resonances hybridize the exciton wave function over four different electron and hole single-particle orbitals. Comparisons of experimental observations with microscopic eight-band k·p calculations taking into account a realistic quantum dot geometry show good agreement and reveal that the Coulomb resonances arise from broken symmetry in the artificial semiconductor molecule.
Hopping mixed hybrid excitations in multiple composite quantum wire structures
International Nuclear Information System (INIS)
Nguyen Ba An; Tran Thai Hoa
1995-10-01
A structure consisting of N pairs of inorganic semiconductor and organic quantum wires is considered theoretically. In such an isolated pair of wires, while the intrawire coupling forms Wannier-Mott exciton in an inorganic semiconductor quantum wire and Frenkel exciton in an organic one, the interwire coupling gives rise to hybrid excitons residing within the pair. When N pairs of wires are packed together 2N new mixed hybrid modes appear that are the true elementary excitations and can hop throughout the whole structure. Energies and wave functions of such hopping mixed hybrid excitations are derived analytically in detail accounting for the global interwire coupling and the different polarization configurations. (author). 19 refs
Nishizawa, Hiroaki; Nishimura, Yoshifumi; Kobayashi, Masato; Irle, Stephan; Nakai, Hiromi
2016-08-05
The linear-scaling divide-and-conquer (DC) quantum chemical methodology is applied to the density-functional tight-binding (DFTB) theory to develop a massively parallel program that achieves on-the-fly molecular reaction dynamics simulations of huge systems from scratch. The functions to perform large scale geometry optimization and molecular dynamics with DC-DFTB potential energy surface are implemented to the program called DC-DFTB-K. A novel interpolation-based algorithm is developed for parallelizing the determination of the Fermi level in the DC method. The performance of the DC-DFTB-K program is assessed using a laboratory computer and the K computer. Numerical tests show the high efficiency of the DC-DFTB-K program, a single-point energy gradient calculation of a one-million-atom system is completed within 60 s using 7290 nodes of the K computer. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.
Tahan, A; Monajjemi, M
2011-12-01
Quantum mechanical and molecular dynamics methods were used to analyze the structure and stability of neutral and zwitterionic configurations of the extracted active site sequence from a Burkholderia cepacia lipase, histidyl-seryl-glutamin (His86-Ser87-Gln88) and its mutated form, histidyl-cysteyl-glutamin (His86-Cys87-Gln88) in vacuum and different solvents. The effects of solvent dielectric constant, explicit and implicit water molecules and side chain mutation on the structure and stability of this sequence in both neutral and zwitterionic forms are represented. The quantum mechanics computations represent that the relative stability of zwitterionic and neutral configurations depends on the solvent structure and its dielectric constant. Therefore, in vacuum and the considered non-polar solvents, the neutral form of the interested sequences is more stable than the zwitterionic form, while their zwitterionic form is more stable than the neutral form in the aqueous solution and the investigated polar solvents in most cases. However, on the potential energy surfaces calculated, there is a barrier to proton transfer from the positively charged ammonium group to the negatively charged carboxylat group or from the ammonium group to the adjacent carbonyl oxygen and or from side chain oxygen and sulfur to negatively charged carboxylat group. Molecular dynamics simulations (MD) were also performed by using periodic boundary conditions for the zwitterionic configuration of the hydrated molecules in a box of water molecules. The obtained results demonstrated that the presence of explicit water molecules provides the more compact structures of the studied molecules. These simulations also indicated that side chain mutation and replacement of sulfur with oxygen leads to reduction of molecular flexibility and packing.
Photoluminescence of hybrid quantum dot systems
Czech Academy of Sciences Publication Activity Database
Král, Karel; Menšík, Miroslav
2015-01-01
Roč. 7, č. 4 (2015), 347-349 ISSN 2164-6627 R&D Projects: GA MŠk LH12236; GA MŠk LH12186 Institutional support: RVO:68378271 ; RVO:61389013 Keywords : quantum dots * energy transfer * electron-phonon interaction Subject RIV: BM - Solid Matter Physics ; Magnetism
Multi-functional quantum router using hybrid opto-electromechanics
Ma, Peng-Cheng; Yan, Lei-Lei; Chen, Gui-Bin; Li, Xiao-Wei; Liu, Shu-Jing; Zhan, You-Bang
2018-03-01
Quantum routers engineered with multiple frequency bands play a key role in quantum networks. We propose an experimentally accessible scheme for a multi-functional quantum router, using photon-phonon conversion in a hybrid opto-electromechanical system. Our proposed device functions as a bidirectional, tunable multi-channel quantum router, and demonstrates the possibility to route single optical photons bidirectionally and simultaneously to three different output ports, by adjusting the microwave power. Further, the device also behaves as an interswitching unit for microwave and optical photons, yielding probabilistic routing of microwave (optical) signals to optical (microwave) outports. With respect to potential application, we verify the insignificant influence from vacuum and thermal noises in the performance of the router under cryogenic conditions.
Wang, Meiting; Li, Pengfei; Jia, Xiangyu; Liu, Wei; Shao, Yihan; Hu, Wenxin; Zheng, Jun; Brooks, Bernard R; Mei, Ye
2017-10-23
The partitioning of solute molecules between immiscible solvents with significantly different polarities is of great importance. The polarization between the solute and solvent molecules plays an essential role in determining the solubility of the solute, which makes computational studies utilizing molecular mechanics (MM) rather difficult. In contrast, quantum mechanics (QM) can provide more reliable predictions. In this work, the partition coefficients of the side chain analogs of some amino acids between water and chloroform were computed. The QM solvation free energies were calculated indirectly via a series of MM states using the multistate Bennett acceptance ratio (MBAR) and the MM-to-QM corrections were applied at the two endpoints using thermodynamic perturbation (TP). Previously, it has been shown (Jia et al. J. Chem. Theory Comput. 2016, 12, 499-511) that this method provides the minimal variance in the results without running QM simulations. However, if there is insufficient overlap in phase space between the MM and QM Hamiltonians, this method fails. In this work, we propose, for the first time, a quantity termed the reweighting entropy that serves as a metric for the reliability of the TP calculations. If the reweighting entropy is below a certain threshold (0.65 for the solvation free energy calculations in this work), this MM-to-QM correction should be avoided and two alternative methods can be employed by either introducing a semiempirical state or conducting nonequilibrium simulations. However, the results show that the QM methods are not guaranteed to yield better results than the MM methods. Further improvement of the QM methods are imperative, especially the treatment of the van der Waals and the electrostatic interactions between the QM region and the MM region in the first shell. We also propose a scheme for the calculation of the van der Waals parameters for the solute molecules in nonaqueous solvent, which improves the quality of the
Towards the experimental realization of hybrid quantum systems
International Nuclear Information System (INIS)
Koller, C.
2012-01-01
One of the main interests of quantum physics in this new millennium is the exploitation of quantum mechanical principles in technical applications. One approach here is to use entanglement and superpositions of states to realize powerful algorithms capable of solving challenging computational tasks on a much faster time scale than a classical computer ever could. To find the quantum analogue of a classical bit one needs a quantum mechanical two level system that can be used to store and process quantum information. Most of the current approaches to find such a 'qubit' have the intention to find a single system that is able to fulfill all desirable tasks. But actually most quantum systems are only favorable for very specific tasks (e.g storage, processing, data exchange,..), similar as it is in classical computing. For some qubits the main disadvantages is that their quantum state is very fragile. Those systems loose their 'quantum information' (that is the possibility to store superpositions of their states coherently) easily. They 'decohere' on a timescale that is much shorter then any more involving algorithm. Other systems can keep those superposition states for quite a while, but are so difficult to address that the number of operations that can be made is very limited. The task of a so called hybrid quantum system is now to combine the strengths of these different systems, using e.g. one for manipulation and an other system for storage. Similar to a processor/memory architecture in conventional computers these systems could use a kind of bus system to couple between them. The main task of this thesis was to make steps towards the realization of such a system using two different combinations of quantum systems. Both are planned to use superconducting qubits (transmons) as processor qubit and either atoms (ultra cold rubidium 87 ensembles) or solid state spin systems (Nitrogen Vacancies in diamonds - NV centers) as memory. (author)
Hybrid Quantum Information Processing with Superconductors and Neutral Atoms
McDermott, Robert
Hybrid approaches to quantum information processing (QIP) aim to capitalize on the strengths of disparate quantum technologies to realize a system whose capabilities exceed those of any single experimental platform. At the University of Wisconsin, we are working toward integration of a fast superconducting quantum processor with a stable, long-lived quantum memory based on trapped neutral atoms. Here we describe the development of a quantum interface between superconducting thin-film cavity circuits and trapped Rydberg atoms, the key technological obstacle to realization of superconductor-atom hybrid QIP. Specific accomplishments to date include development of a theoretical protocol for high-fidelity state transfer between the atom and the cavity; fabrication and characterization of high- Q superconducting cavities with integrated trapping electrodes to enhance zero-point microwave fields at a location remote from the chip surface; and trapping and Rydberg excitation of single atoms within 1 mm of the cavity. We discuss the status of experiments to probe the strong coherent coupling of single Rydberg atoms and the superconducting cavity. Supported by ARO under contract W911NF-16-1-0133.
Quantum Efficiency of Hybrid Photon Detectors for the LHCb RICH
Lambert, R W
2008-01-01
The production of Hybrid Photon Detectors to be used as the single-photon sensors for the RICH detectors of the LHCb experiment has recently finished. We present the quantum efficiency measurements of the entire sample of 550 tubes. The manufacturer has succeeded in consistently improving the quantum efficiency of the employed S20-type multi-alkali photocathode above our expectations, by a relative 27 % integrated over the energy spectrum. We also report measurements of the vacuum quality using the photocurrent of the device as a monitor for possible vacuum degradation.
Thomas, Laura L; Tirado-Rives, Julian; Jorgensen, William L
2010-03-10
Quantum and molecular mechanics calculations for the Diels-Alder reactions of cyclopentadiene with 1,4-naphthoquinone, methyl vinyl ketone, and acrylonitrile have been carried out at the vacuum-water interface and in the gas phase. In conjunction with previous studies of these cycloadditions in dilute solution, a more complete picture of aqueous environmental effects emerges with implications for the origin of observed rate accelerations using heterogeneous aqueous suspensions, "on water" conditions. The pure TIP4P water slab maintains the bulk density and hydrogen-bonding properties in central water layers. The bulk region merges to vacuum over a ca. 5 A band with progressive diminution of the density and hydrogen bonding. The relative free energies of activation and transition structures for the reactions at the interface are found to be intermediate between those calculated in the gas phase and in bulk water; i.e., for the reaction with 1,4-naphthoquinone, the DeltaDeltaG(++) values relative to the gas phase are -3.6 and -7.3 kcal/mol at the interface and in bulk water, respectively. Thus, the results do not support the notion that a water surface is more effective than bulk water for catalysis of such pericyclic reactions. The trend is in qualitative agreement with expectations based on density considerations and estimates of experimental rate constants for the gas phase, a heterogeneous aqueous suspension, and a dilute aqueous solution for the reaction of cyclopentadiene with methyl vinyl ketone. Computed energy pair distributions reveal a uniform loss of 0.5-1.0 hydrogen bond for the reactants and transition states in progressing from bulk water to the vacuum-water interface. Orientational effects are apparent at the surface; e.g., the carbonyl group in the methyl vinyl ketone transition structure is preferentially oriented into the surface. Also, the transition structure for the 1,4-naphthoquinone case is buried more in the surface, and the free energy of
Narzi, Daniele; Capone, Matteo; Bovi, Daniele; Guidoni, Leonardo
2018-04-16
Water oxidation in the early steps of natural photosynthesis is fulfilled by photosystem II, which is a protein complex embedded in the thylakoid membrane inside chloroplasts. The water oxidation reaction occurs in the catalytic core of photosystem II, which consists of a Mn4Ca metal cluster, at which, after the accumulation of four oxidising equivalents through five steps (S0-S4) of the Kok-Joliot cycle, two water molecules are split into electrons, protons, and molecular oxygen. In recent years, by combining experimental and theoretical approaches, new insights have been achieved into the structural and electronic properties of different steps of the catalytic cycle. Nevertheless, the exact catalytic mechanism, especially concerning the final stages of the cycle, remains elusive and greatly debated. Herein, by means of quantum mechanics/molecular mechanics (QM/MM) molecular dynamics simulations, from the structural, electronic, and magnetic points of view, the S 3 state before and upon oxidation has been characterised. In contrast with the S 2 state, the oxidation of the S 3 state is not followed by a spontaneous proton-coupled electron-transfer event. Nevertheless, upon modelling the reduction of the tyrosine residue in photosystem II (Tyr Z ) and the protonation of Asp61, spontaneous proton transfer occurs, leading to the deprotonation of an oxygen atom bound to Mn1; thus making it available for O-O bond formation. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Yao, Jianzhuang; Wang, Xia; Luo, Haixia; Gu, Pengfei
2017-11-16
Shikimate kinase (SK) is the fifth bacterial enzyme involved in the shikimate pathway for biosynthesis of life-indispensable components, such as aromatic amino acids. The absence of the shikimate pathway in humans makes SK an attractive target for the rational design of drugs aimed at pathogenesis bacteria, such as Mycobacterium tuberculosis and Helicobacter pylori. However, an effective inhibitor of SK (e.g., a transition-state analogue) is still not available on the market due, at least in part, to a lack of knowledge on the catalytic mechanism and the nature of the rate-limiting transition state. Herein, quantum mechanical/molecular mechanical (QM/MM) reaction coordinate, molecular dynamics (MD), and free-energy simulations have been performed to answer these questions. The results presented herein demonstrate that the phosphoryl-transfer process, which is the rate-limiting step of SK-catalyzed phosphorylation of shikimic acid (SKM), is a concerted one-step reaction proceeding through a loose transition state. The computational results agree well with those of experimental studies, specifically NMR results, X-ray crystal structure observation, and activation free-energy barrier. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Takahashi, Hideaki; Ohno, Hajime; Kishi, Ryohei; Nakano, Masayoshi; Matubayasi, Nobuyuki
2008-11-28
The isoalloxazine ring (flavin ring) is a part of the coenzyme flavin adenine dinucleotide and acts as an active site in the oxidation of a substrate. We have computed the free energy change Deltamicro(red) associated with one-electron reduction of the flavin ring immersed in water by utilizing the quantum mechanical/molecular mechanical method combined with the theory of energy representation (QM/MM-ER method) recently developed. As a novel treatment in implementing the QM/MM-ER method, we have identified the excess charge to be attached on the flavin ring as a solute while the remaining molecules, i.e., flavin ring and surrounding water molecules, are treated as solvent species. Then, the reduction free energy can be decomposed into the contribution Deltamicro(red)(QM) due to the oxidant described quantum chemically and the free energy Deltamicro(red)(MM) due to the water molecules represented by a classical model. By the sum of these contributions, the total reduction free energy Deltamicro(red) has been given as -80.1 kcal/mol. To examine the accuracy and efficiency of this approach, we have also conducted the Deltamicro(red) calculation using the conventional scheme that Deltamicro(red) is constructed from the solvation free energies of the flavin rings at the oxidized and reduced states. The conventional scheme has been implemented with the QM/MM-ER method and the calculated Deltamicro(red) has been estimated as -81.0 kcal/mol, showing excellent agreement with the value given by the new approach. The present approach is efficient, in particular, to compute free energy change for the reaction occurring in a protein since it enables ones to circumvent the numerical problem brought about by subtracting the huge solvation free energies of the proteins in two states before and after the reduction.
Fluorescence from a quantum dot and metallic nanosphere hybrid system
Energy Technology Data Exchange (ETDEWEB)
Schindel, Daniel G. [Department of Mathematics and Statistics, University of Winnipeg, 515 Portage Avenue, Winnipeg, MB, R3B 2E9 (Canada); Singh, Mahi R. [Department of Physics and Astronomy, University of Western Ontario, 1151 Richmond Street, London, ON, N6A 3K7 (Canada)
2014-03-31
We present energy absorption and interference in a quantum dot-metallic nanosphere system embedded on a dielectric substrate. A control field is applied to induce dipole moments in the nanosphere and the quantum dot, and a probe field is applied to monitor absorption. Dipole moments in the quantum dot or the metal nanosphere are induced, both by the external fields and by each other's dipole fields. Thus, in addition to direct polarization, the metal nanosphere and the quantum dot will sense one another via the dipole-dipole interaction. The density matrix method was used to show that the absorption spectrum can be split from one peak to two peaks by the control field, and this can also be done by placing the metal sphere close to the quantum dot. When the two are extremely close together, a self-interaction in the quantum dot produces an asymmetry in the absorption peaks. In addition, the fluorescence efficiency can be quenched by the addition of a metal nanosphere. This hybrid system could be used to create ultra-fast switching and sensing nanodevices.
Valley-orbit hybrid states in Si quantum dots
Gamble, John; Friesen, Mark; Coppersmith, S. N.
2013-03-01
The conduction band for electrons in layered Si nanostructures oriented along (001) has two low-lying valleys. Most theoretical treatments assume that these valleys are decoupled from the long-wavelength physics of electron confinement. In this work, we show that even a minimal amount of disorder (a single atomic step at the quantum well interface) is sufficient to mix valley states and electron orbitals, causing a significant distortion of the long-wavelength electron envelope. For physically realistic electric fields and dot sizes, this valley-orbit coupling impacts all electronic states in Si quantum dots, implying that one must always consider valley-orbit hybrid states, rather than distinct valley and orbital degrees of freedom. We discuss the ramifications of our results on silicon quantum dot qubits. This work was supported in part by ARO (W911NF-08-1-0482) and NSF (DMR-0805045).
Quantum control and process tomography of a semiconductor quantum dot hybrid qubit.
Kim, Dohun; Shi, Zhan; Simmons, C B; Ward, D R; Prance, J R; Koh, Teck Seng; Gamble, John King; Savage, D E; Lagally, M G; Friesen, Mark; Coppersmith, S N; Eriksson, Mark A
2014-07-03
The similarities between gated quantum dots and the transistors in modern microelectronics--in fabrication methods, physical structure and voltage scales for manipulation--have led to great interest in the development of quantum bits (qubits) in semiconductor quantum dots. Although quantum dot spin qubits have demonstrated long coherence times, their manipulation is often slower than desired for important future applications, such as factoring. Furthermore, scalability and manufacturability are enhanced when qubits are as simple as possible. Previous work has increased the speed of spin qubit rotations by making use of integrated micromagnets, dynamic pumping of nuclear spins or the addition of a third quantum dot. Here we demonstrate a qubit that is a hybrid of spin and charge. It is simple, requiring neither nuclear-state preparation nor micromagnets. Unlike previous double-dot qubits, the hybrid qubit enables fast rotations about two axes of the Bloch sphere. We demonstrate full control on the Bloch sphere with π-rotation times of less than 100 picoseconds in two orthogonal directions, which is more than an order of magnitude faster than any other double-dot qubit. The speed arises from the qubit's charge-like characteristics, and its spin-like features result in resistance to decoherence over a wide range of gate voltages. We achieve full process tomography in our electrically controlled semiconductor quantum dot qubit, extracting high fidelities of 85 per cent for X rotations (transitions between qubit states) and 94 per cent for Z rotations (phase accumulation between qubit states).
Nakamura, Shin; Ota, Kai; Shibuya, Yuichi; Noguchi, Takumi
2016-01-26
Photosynthetic water oxidation takes place at the Mn4CaO5 cluster in photosystem II. Around the Mn4CaO5 cluster, a hydrogen bond network is formed by several water molecules, including four water ligands. To clarify the role of this water network in the mechanism of water oxidation, we investigated the effects of the removal of Ca(2+) and substitution with metal ions on the vibrations of water molecules coupled to the Mn4CaO5 cluster by means of Fourier transform infrared (FTIR) difference spectroscopy and quantum mechanics/molecular mechanics (QM/MM) calculations. The OH stretching vibrations of nine water molecules forming a network between D1-D61 and YZ were calculated using the QM/MM method. On the the calculated normal modes, a broad positive feature at 3200-2500 cm(-1) in an S2-minus-S1 FTIR spectrum was attributed to the vibrations of strongly hydrogen-bonded OH bonds of water involving the vibrations of water ligands to a Mn ion and the in-phase coupled vibration of a water network connected to YZ, while bands in the 3700-3500 cm(-1) region were assigned to the coupled vibrations of weakly hydrogen-bonded OH bonds of water. All the water bands were lost upon Ca(2+) depletion and Ba(2+) substitution, which inhibit the S2 → S3 transition, indicating that a solid water network was broken by these treatments. By contrast, Sr(2+) substitution slightly altered the water bands around 3600 cm(-1), reflecting minor modification in water interactions, consistent with the retention of water oxidation activity with a decreased efficiency. These results suggest that the water network around the Mn4CaO5 cluster plays an essential role in the water oxidation mechanism particularly in a concerted process of proton transfer and water insertion during the S2 → S3 transition.
Micropatterned superconducting film circuitry for operation in hybrid quantum devices
International Nuclear Information System (INIS)
Bothner, Daniel
2013-01-01
This thesis discusses three aspects of the arduous way towards hybrid quantum systems consisting of superconducting circuits and ensembles of ultracold paramagnetic atoms. In the first part of the thesis, superconducting coplanar microwave resonators as used for quantum information processing with superconducting qubits are investigated in magnetic fields. In the second part of the thesis integrated atom chips are designed and fabricated, which offer the possibility to trap an ensemble of ultracold atoms close to a superconducting coplanar resonator on that chip. In the third and last part of the thesis, unconventional disordered and quasiperiodic arrangements of microfabricated holes (antidots) in superconducting films are patterned and investigated with respect to the impact of the arrangement on the superconductor transport properties in magnetic fields.
Hybrid classical/quantum simulation for infrared spectroscopy of water
Maekawa, Yuki; Sasaoka, Kenji; Ube, Takuji; Ishiguro, Takashi; Yamamoto, Takahiro
2018-05-01
We have developed a hybrid classical/quantum simulation method to calculate the infrared (IR) spectrum of water. The proposed method achieves much higher accuracy than conventional classical molecular dynamics (MD) simulations at a much lower computational cost than ab initio MD simulations. The IR spectrum of water is obtained as an ensemble average of the eigenvalues of the dynamical matrix constructed by ab initio calculations, using the positions of oxygen atoms that constitute water molecules obtained from the classical MD simulation. The calculated IR spectrum is in excellent agreement with the experimental IR spectrum.
Microscale memory characteristics of virus-quantum dot hybrids
Portney, Nathaniel G.; Tseng, Ricky J.; Destito, Giuseppe; Strable, Erica; Yang, Yang; Manchester, Marianne; Finn, M. G.; Ozkan, Mihrimah
2007-05-01
An electrical multi stability effect was observed for a single layer device fabricated, comprising a hybrid virus-semiconducting quantum dot (CdSe /ZnS core/shell Qds) assembled onto icosahedral-mutant-virus template (CPMV-T184C). A substrate based bottom-up pathway was used to conjugate two different color emitting Qds for fluorescence visualization and to insert a charging/decharging factor. Pulsed wave measurements depicted distinct conductive states with repeatable and nonvolatile behavior as a functioning memory element.
Self-assembling hybrid diamond–biological quantum devices
International Nuclear Information System (INIS)
Albrecht, A; B Plenio, M; Koplovitz, G; Yochelis, S; Paltiel, Y; Retzker, A; Nevo, Y; Shoseyov, O; Jelezko, F; Porath, D
2014-01-01
The realization of scalable arrangements of nitrogen vacancy (NV) centers in diamond remains a key challenge on the way towards efficient quantum information processing, quantum simulation and quantum sensing applications. Although technologies based on implanting NV-centers in bulk diamond crystals or hybrid device approaches have been developed, they are limited by the achievable spatial resolution and by the intricate technological complexities involved in achieving scalability. We propose and demonstrate a novel approach for creating an arrangement of NV-centers, based on the self-assembling capabilities of biological systems and their beneficial nanometer spatial resolution. Here, a self-assembled protein structure serves as a structural scaffold for surface functionalized nanodiamonds, in this way allowing for the controlled creation of NV-structures on the nanoscale and providing a new avenue towards bridging the bio–nano interface. One-, two- as well as three-dimensional structures are within the scope of biological structural assembling techniques. We realized experimentally the formation of regular structures by interconnecting nanodiamonds using biological protein scaffolds. Based on the achievable NV-center distances of 11 nm, we evaluate the expected dipolar coupling interaction with neighboring NV-centers as well as the expected decoherence time. Moreover, by exploiting these couplings, we provide a detailed theoretical analysis on the viability of multiqubit quantum operations, suggest the possibility of individual addressing based on the random distribution of the NV intrinsic symmetry axes and address the challenges posed by decoherence and imperfect couplings. We then demonstrate in the last part that our scheme allows for the high-fidelity creation of entanglement, cluster states and quantum simulation applications. (papers)
Self-assembling hybrid diamond-biological quantum devices
Albrecht, A.; Koplovitz, G.; Retzker, A.; Jelezko, F.; Yochelis, S.; Porath, D.; Nevo, Y.; Shoseyov, O.; Paltiel, Y.; Plenio, M. B.
2014-09-01
The realization of scalable arrangements of nitrogen vacancy (NV) centers in diamond remains a key challenge on the way towards efficient quantum information processing, quantum simulation and quantum sensing applications. Although technologies based on implanting NV-centers in bulk diamond crystals or hybrid device approaches have been developed, they are limited by the achievable spatial resolution and by the intricate technological complexities involved in achieving scalability. We propose and demonstrate a novel approach for creating an arrangement of NV-centers, based on the self-assembling capabilities of biological systems and their beneficial nanometer spatial resolution. Here, a self-assembled protein structure serves as a structural scaffold for surface functionalized nanodiamonds, in this way allowing for the controlled creation of NV-structures on the nanoscale and providing a new avenue towards bridging the bio-nano interface. One-, two- as well as three-dimensional structures are within the scope of biological structural assembling techniques. We realized experimentally the formation of regular structures by interconnecting nanodiamonds using biological protein scaffolds. Based on the achievable NV-center distances of 11 nm, we evaluate the expected dipolar coupling interaction with neighboring NV-centers as well as the expected decoherence time. Moreover, by exploiting these couplings, we provide a detailed theoretical analysis on the viability of multiqubit quantum operations, suggest the possibility of individual addressing based on the random distribution of the NV intrinsic symmetry axes and address the challenges posed by decoherence and imperfect couplings. We then demonstrate in the last part that our scheme allows for the high-fidelity creation of entanglement, cluster states and quantum simulation applications.
A hybrid plasmonic waveguide terahertz quantum cascade laser
Energy Technology Data Exchange (ETDEWEB)
Degl' Innocenti, Riccardo, E-mail: rd448@cam.ac.uk; Shah, Yash D.; Wallis, Robert; Klimont, Adam; Ren, Yuan; Jessop, David S.; Beere, Harvey E.; Ritchie, David A. [Cavendish Laboratory, University of Cambridge, J. J. Thomson Avenue, Cambridge CB3 0HE (United Kingdom)
2015-02-23
We present the realization of a quantum cascade laser emitting at around 2.85 THz, based on a hybrid plasmonic waveguide with a low refractive index dielectric cladding. This hybrid waveguide design allows the performance of a double-metal waveguide to be retained, while improving the emission far-field. A set of lasers based on the same active region material were fabricated with different metal layer thicknesses. A detailed characterization of the performance of these lasers revealed that there is an optimal trade-off that yields the best far-field emission and the maximum temperature of operation. By exploiting the pure plasmonic mode of these waveguides, the standard operation conditions of a double-metal quantum cascade laser were retrieved, such that the maximum operating temperature of these devices is not affected by the process. These results pave the way to realizing a class of integrated devices working in the terahertz range which could be further exploited to fabricate terahertz on-chip circuitry.
Quantum dot-dye hybrid systems for energy transfer applications
International Nuclear Information System (INIS)
Ren, Ting
2010-01-01
In this thesis, we focus on the preparation of energy transfer-based quantum dot (QD)-dye hybrid systems. Two kinds of QD-dye hybrid systems have been successfully synthesized: QD-silica-dye and QD-dye hybrid systems. In the QD-silica-dye hybrid system, multishell CdSe/CdS/ZnS QDs were adsorbed onto monodisperse Stoeber silica particles with an outer silica shell of thickness 2-24 nm containing organic dye molecules (Texas Red). The thickness of this dye layer has a strong effect on the total sensitized acceptor emission, which is explained by the increase in the number of dye molecules homogeneously distributed within the silica shell, in combination with an enhanced surface adsorption of QDs with increasing dye amount. Our conclusions were underlined by comparison of the experimental results with Monte-Carlo simulations, and by control experiments confirming attractive interactions between QDs and Texas Red freely dissolved in solution. New QD-dye hybrid system consisting of multishell QDs and organic perylene dyes have been synthesized. We developed a versatile approach to assemble extraordinarily stable QD-dye hybrids, which uses dicarboxylate anchors to bind rylene dyes to QD. This system yields a good basis to study the energy transfer between QD and dye because of its simple and compact design: there is no third kind of molecule linking QD and dye; no spacer; and the affinity of the functional group to the QD surface is strong. The FRET signal was measured for these complexes as a function of both dye to QD ratio and center-to-center distance between QD and dye by controlling number of covered ZnS layers. Data showed that fluorescence resonance energy transfer (FRET) was the dominant mechanism of the energy transfer in our QD-dye hybrid system. FRET efficiency can be controlled by not only adjusting the number of dyes on the QD surface or the QD to dye distance, but also properly choosing different dye and QD components. Due to the strong stability, our QD
Quantum dot-dye hybrid systems for energy transfer applications
Energy Technology Data Exchange (ETDEWEB)
Ren, Ting
2010-07-01
In this thesis, we focus on the preparation of energy transfer-based quantum dot (QD)-dye hybrid systems. Two kinds of QD-dye hybrid systems have been successfully synthesized: QD-silica-dye and QD-dye hybrid systems. In the QD-silica-dye hybrid system, multishell CdSe/CdS/ZnS QDs were adsorbed onto monodisperse Stoeber silica particles with an outer silica shell of thickness 2-24 nm containing organic dye molecules (Texas Red). The thickness of this dye layer has a strong effect on the total sensitized acceptor emission, which is explained by the increase in the number of dye molecules homogeneously distributed within the silica shell, in combination with an enhanced surface adsorption of QDs with increasing dye amount. Our conclusions were underlined by comparison of the experimental results with Monte-Carlo simulations, and by control experiments confirming attractive interactions between QDs and Texas Red freely dissolved in solution. New QD-dye hybrid system consisting of multishell QDs and organic perylene dyes have been synthesized. We developed a versatile approach to assemble extraordinarily stable QD-dye hybrids, which uses dicarboxylate anchors to bind rylene dyes to QD. This system yields a good basis to study the energy transfer between QD and dye because of its simple and compact design: there is no third kind of molecule linking QD and dye; no spacer; and the affinity of the functional group to the QD surface is strong. The FRET signal was measured for these complexes as a function of both dye to QD ratio and center-to-center distance between QD and dye by controlling number of covered ZnS layers. Data showed that fluorescence resonance energy transfer (FRET) was the dominant mechanism of the energy transfer in our QD-dye hybrid system. FRET efficiency can be controlled by not only adjusting the number of dyes on the QD surface or the QD to dye distance, but also properly choosing different dye and QD components. Due to the strong stability, our QD
Gauge-invariant perturbations in hybrid quantum cosmology
Energy Technology Data Exchange (ETDEWEB)
Gomar, Laura Castelló; Marugán, Guillermo A. Mena [Instituto de Estructura de la Materia, CSIC, Serrano 121, 28006 Madrid (Spain); Martín-Benito, Mercedes, E-mail: laura.castello@iem.cfmac.csic.es, E-mail: m.martin@hef.ru.nl, E-mail: mena@iem.cfmac.csic.es [Institute for Mathematics, Astrophysics and Particle Physics, Radboud University Nijmegen, Heyendaalseweg 135, NL-6525 AJ Nijmegen (Netherlands)
2015-06-01
We consider cosmological perturbations around homogeneous and isotropic spacetimes minimally coupled to a scalar field and present a formulation which is designed to preserve covariance. We truncate the action at quadratic perturbative order and particularize our analysis to flat compact spatial sections and a field potential given by a mass term, although the formalism can be extended to other topologies and potentials. The perturbations are described in terms of Mukhanov-Sasaki gauge invariants, linear perturbative constraints, and variables canonically conjugate to them. This set is completed into a canonical one for the entire system, including the homogeneous degrees of freedom. We find the global Hamiltonian constraint of the model, in which the contribution of the homogeneous sector is corrected with a term quadratic in the perturbations, that can be identified as the Mukhanov-Sasaki Hamiltonian in our formulation. We then adopt a hybrid approach to quantize the model, combining a quantum representation of the homogeneous sector with a more standard field quantization of the perturbations. Covariance is guaranteed in this approach inasmuch as no gauge fixing is adopted. Next, we adopt a Born-Oppenheimer ansatz for physical states and show how to obtain a Schrödinger-like equation for the quantum evolution of the perturbations. This evolution is governed by the Mukhanov-Sasaki Hamiltonian, with the dependence on the homogeneous geometry evaluated at quantum expectation values, and with a time parameter defined also in terms of suitable expectation values on that geometry. Finally, we derive effective equations for the dynamics of the Mukhanov-Sasaki gauge invariants, that include quantum contributions, but have the same ultraviolet limit as the classical equations. They provide the master equation to extract predictions about the power spectrum of primordial scalar perturbations.
Gauge-invariant perturbations in hybrid quantum cosmology
International Nuclear Information System (INIS)
Gomar, Laura Castelló; Marugán, Guillermo A. Mena; Martín-Benito, Mercedes
2015-01-01
We consider cosmological perturbations around homogeneous and isotropic spacetimes minimally coupled to a scalar field and present a formulation which is designed to preserve covariance. We truncate the action at quadratic perturbative order and particularize our analysis to flat compact spatial sections and a field potential given by a mass term, although the formalism can be extended to other topologies and potentials. The perturbations are described in terms of Mukhanov-Sasaki gauge invariants, linear perturbative constraints, and variables canonically conjugate to them. This set is completed into a canonical one for the entire system, including the homogeneous degrees of freedom. We find the global Hamiltonian constraint of the model, in which the contribution of the homogeneous sector is corrected with a term quadratic in the perturbations, that can be identified as the Mukhanov-Sasaki Hamiltonian in our formulation. We then adopt a hybrid approach to quantize the model, combining a quantum representation of the homogeneous sector with a more standard field quantization of the perturbations. Covariance is guaranteed in this approach inasmuch as no gauge fixing is adopted. Next, we adopt a Born-Oppenheimer ansatz for physical states and show how to obtain a Schrödinger-like equation for the quantum evolution of the perturbations. This evolution is governed by the Mukhanov-Sasaki Hamiltonian, with the dependence on the homogeneous geometry evaluated at quantum expectation values, and with a time parameter defined also in terms of suitable expectation values on that geometry. Finally, we derive effective equations for the dynamics of the Mukhanov-Sasaki gauge invariants, that include quantum contributions, but have the same ultraviolet limit as the classical equations. They provide the master equation to extract predictions about the power spectrum of primordial scalar perturbations
A hybrid-type quantum random number generator
Hai-Qiang, Ma; Wu, Zhu; Ke-Jin, Wei; Rui-Xue, Li; Hong-Wei, Liu
2016-05-01
This paper proposes a well-performing hybrid-type truly quantum random number generator based on the time interval between two independent single-photon detection signals, which is practical and intuitive, and generates the initial random number sources from a combination of multiple existing random number sources. A time-to-amplitude converter and multichannel analyzer are used for qualitative analysis to demonstrate that each and every step is random. Furthermore, a carefully designed data acquisition system is used to obtain a high-quality random sequence. Our scheme is simple and proves that the random number bit rate can be dramatically increased to satisfy practical requirements. Project supported by the National Natural Science Foundation of China (Grant Nos. 61178010 and 11374042), the Fund of State Key Laboratory of Information Photonics and Optical Communications (Beijing University of Posts and Telecommunications), China, and the Fundamental Research Funds for the Central Universities of China (Grant No. bupt2014TS01).
Memory-built-in quantum cloning in a hybrid solid-state spin register
Wang, W.-B.; Zu, C.; He, L.; Zhang, W.-G.; Duan, L.-M.
2015-07-01
As a way to circumvent the quantum no-cloning theorem, approximate quantum cloning protocols have received wide attention with remarkable applications. Copying of quantum states to memory qubits provides an important strategy for eavesdropping in quantum cryptography. We report an experiment that realizes cloning of quantum states from an electron spin to a nuclear spin in a hybrid solid-state spin register with near-optimal fidelity. The nuclear spin provides an ideal memory qubit at room temperature, which stores the cloned quantum states for a millisecond under ambient conditions, exceeding the lifetime of the original quantum state carried by the electron spin by orders of magnitude. The realization of a cloning machine with built-in quantum memory provides a key step for application of quantum cloning in quantum information science.
Monolithic Hybrid and Passive Mode-Locked 40GHz Quantum Dot Laser Diodes
DEFF Research Database (Denmark)
Thompson, M. G.; Larsson, David; Rae, A. R.
2006-01-01
For the first time hybrid and passive mode-locking jitter performance is investigated in 40GHz quantum-dot mode-locked lasers. Record low passive mode-locking jitter of 219fs is presented, along with promising hybrid mode-locking results of 124fs.......For the first time hybrid and passive mode-locking jitter performance is investigated in 40GHz quantum-dot mode-locked lasers. Record low passive mode-locking jitter of 219fs is presented, along with promising hybrid mode-locking results of 124fs....
Askerka, Mikhail; Brudvig, Gary W; Batista, Victor S
2017-01-17
Efficient photoelectrochemical water oxidation may open a way to produce energy from renewable solar power. In biology, generation of fuel due to water oxidation happens efficiently on an immense scale during the light reactions of photosynthesis. To oxidize water, photosynthetic organisms have evolved a highly conserved protein complex, Photosystem II. Within that complex, water oxidation happens at the CaMn 4 O 5 inorganic catalytic cluster, the so-called oxygen-evolving complex (OEC), which cycles through storage "S" states as it accumulates oxidizing equivalents and produces molecular oxygen. In recent years, there has been significant progress in understanding the OEC as it evolves through the catalytic cycle. Studies have combined conventional and femtosecond X-ray crystallography with extended X-ray absorption fine structure (EXAFS) and quantum mechanics/molecular mechanics (QM/MM) methods and have addressed changes in protonation states of μ-oxo bridges and the coordination of substrate water through the analysis of ammonia binding as a chemical analog of water. These advances are thought to be critical to understanding the catalytic cycle since protonation states regulate the relative stability of different redox states and the geometry of the OEC. Therefore, establishing the mechanism for substrate water binding and the nature of protonation/redox state transitions in the OEC is essential for understanding the catalytic cycle of O 2 evolution. The structure of the dark-stable S 1 state has been a target for X-ray crystallography for the past 15 years. However, traditional X-ray crystallography has been hampered by radiation-induced reduction of the OEC. Very recently, a revolutionary X-ray free electron laser (XFEL) technique was applied to PSII to reveal atomic positions at 1.95 Å without radiation damage, which brought us closer than ever to establishing the ultimate structure of the OEC in the S 1 state. However, the atom positions in this crystal
Higher-order spin and charge dynamics in a quantum dot-lead hybrid system.
Otsuka, Tomohiro; Nakajima, Takashi; Delbecq, Matthieu R; Amaha, Shinichi; Yoneda, Jun; Takeda, Kenta; Allison, Giles; Stano, Peter; Noiri, Akito; Ito, Takumi; Loss, Daniel; Ludwig, Arne; Wieck, Andreas D; Tarucha, Seigo
2017-09-22
Understanding the dynamics of open quantum systems is important and challenging in basic physics and applications for quantum devices and quantum computing. Semiconductor quantum dots offer a good platform to explore the physics of open quantum systems because we can tune parameters including the coupling to the environment or leads. Here, we apply the fast single-shot measurement techniques from spin qubit experiments to explore the spin and charge dynamics due to tunnel coupling to a lead in a quantum dot-lead hybrid system. We experimentally observe both spin and charge time evolution via first- and second-order tunneling processes, and reveal the dynamics of the spin-flip through the intermediate state. These results enable and stimulate the exploration of spin dynamics in dot-lead hybrid systems, and may offer useful resources for spin manipulation and simulation of open quantum systems.
Hybrid tandem quantum dot/organic photovoltaic cells with complementary near infrared absorption
Kim, Taesoo; Palmiano, Elenita; Liang, Ru-Ze; Hu, Hanlin; Banavoth, Murali; Kirmani, Ahmad R.; Firdaus, Yuliar; Gao, Yangqin; Sheikh, Arif D.; Yuan, Mingjian; Mohammed, Omar F.; Hoogland, Sjoerd; Beaujuge, Pierre; Sargent, Edward H.; Amassian, Aram
2017-01-01
Monolithically integrated hybrid tandem solar cells that effectively combine solution-processed colloidal quantum dot (CQD) and organic bulk heterojunction subcells to achieve tandem performance that surpasses the individual subcell efficiencies
Hybrid confocal Raman fluorescence microscopy on single cells using semiconductor quantum dots
van Manen, H.J.; Otto, Cornelis
2007-01-01
We have overcome the traditional incompatibility of Raman microscopy with fluorescence microscopy by exploiting the optical properties of semiconductor fluorescent quantum dots (QDs). Here we present a hybrid Raman fluorescence spectral imaging approach for single-cell microscopy applications. We
DEFF Research Database (Denmark)
Aidas, Kestutis; Mikkelsen, Kurt V; Kongsted, Jacob
2010-01-01
The (15)N NMR spectrum of adenine in aqueous solution has been modeled using high-level combined density functional theory/molecular mechanics techniques coupled to a dynamical averaging scheme. The explicit consideration of the three lowest-energy tautomers of adenine-H9, H7 and H3-allows...
Wannier-Frenkel hybrid exciton in organic-semiconductor quantum dot heterostructures
International Nuclear Information System (INIS)
Birman, Joseph L.; Huong, Nguyen Que
2007-01-01
The formation of a hybridization state of Wannier Mott exciton and Frenkel exciton in different hetero-structure configurations involving quantum dots is investigated. The hybrid excitons exist at the interfaces of the semiconductors quantum dots and the organic medium, having unique properties and a large optical non-linearity. The coupling at resonance is very strong and tunable by changing the parameters of the systems (dot radius, dot-dot distance, generation of the organic dendrites and the materials of the system etc...). Different semiconductor quantum dot-organic material combination systems have been considered such as a semiconductor quantum dot lattice embedded in an organic host, a semiconductor quantum dot at the center of an organic dendrite, a semiconductor quantum dot coated by an organic shell
Deterministic linear-optics quantum computing based on a hybrid approach
International Nuclear Information System (INIS)
Lee, Seung-Woo; Jeong, Hyunseok
2014-01-01
We suggest a scheme for all-optical quantum computation using hybrid qubits. It enables one to efficiently perform universal linear-optical gate operations in a simple and near-deterministic way using hybrid entanglement as off-line resources
Deterministic linear-optics quantum computing based on a hybrid approach
Energy Technology Data Exchange (ETDEWEB)
Lee, Seung-Woo; Jeong, Hyunseok [Center for Macroscopic Quantum Control, Department of Physics and Astronomy, Seoul National University, Seoul, 151-742 (Korea, Republic of)
2014-12-04
We suggest a scheme for all-optical quantum computation using hybrid qubits. It enables one to efficiently perform universal linear-optical gate operations in a simple and near-deterministic way using hybrid entanglement as off-line resources.
Photovoltaic Performance of a Nanowire/Quantum Dot Hybrid Nanostructure Array Solar Cell.
Wu, Yao; Yan, Xin; Zhang, Xia; Ren, Xiaomin
2018-02-23
An innovative solar cell based on a nanowire/quantum dot hybrid nanostructure array is designed and analyzed. By growing multilayer InAs quantum dots on the sidewalls of GaAs nanowires, not only the absorption spectrum of GaAs nanowires is extended by quantum dots but also the light absorption of quantum dots is dramatically enhanced due to the light-trapping effect of the nanowire array. By incorporating five layers of InAs quantum dots into a 500-nm high-GaAs nanowire array, the power conversion efficiency enhancement induced by the quantum dots is six times higher than the power conversion efficiency enhancement in thin-film solar cells which contain the same amount of quantum dots, indicating that the nanowire array structure can benefit the photovoltaic performance of quantum dot solar cells.
Graphene and PbS quantum dot hybrid vertical phototransistor
Song, Xiaoxian; Zhang, Yating; Zhang, Haiting; Yu, Yu; Cao, Mingxuan; Che, Yongli; Dai, Haitao; Yang, Junbo; Ding, Xin; Yao, Jianquan
2017-04-01
A field-effect phototransistor based on a graphene and lead sulfide quantum dot (PbS QD) hybrid in which PbS QDs are embedded in a graphene matrix has been fabricated with a vertical architecture through a solution process. The n-type Si/SiO2 substrate (gate), Au/Ag nanowire transparent source electrode, active layer and Au drain electrode are vertically stacked in the device, which has a downscaled channel length of 250 nm. Photoinduced electrons in the PbS QDs leap into the conduction band and fill in the trap states, while the photoinduced holes left in the valence band transfer to the graphene and form the photocurrent under biases from which the photoconductive gain is evaluated. The graphene/QD-based vertical phototransistor shows a photoresponsivity of 2 × 103 A W-1, and specific detectivity up to 7 × 1012 Jones under 808 nm laser illumination with a light irradiance of 12 mW cm-2. The solution-processed vertical phototransistor provides a new facile method for optoelectronic device applications.
Hybrid Approach To Steganography System Based On Quantum Encryption And Chaos Algorithms
Directory of Open Access Journals (Sweden)
ZAID A. ABOD
2018-01-01
Full Text Available A hybrid scheme for secretly embedding image into a dithered multilevel image is presented. This work inputs both a cover image and secret image, which are scrambling and divided into groups to embedded together based on multiple chaos algorithms (Lorenz map, Henon map and Logistic map respectively. Finally, encrypt the embedded images by using one of the quantum cryptography mechanisms, which is quantum one time pad. The experimental results show that the proposed hybrid system successfully embedded images and combine with the quantum cryptography algorithms and gives high efficiency for secure communication.
Optical response of a quantum dot-metal nanoparticle hybrid interacting with a weak probe field.
Kosionis, Spyridon G; Terzis, Andreas F; Sadeghi, Seyed M; Paspalakis, Emmanuel
2013-01-30
We study optical effects in a hybrid system composed of a semiconductor quantum dot and a spherical metal nanoparticle that interacts with a weak probe electromagnetic field. We use modified nonlinear density matrix equations for the description of the optical properties of the system and obtain a closed-form expression for the linear susceptibilities of the quantum dot, the metal nanoparticle, and the total system. We then investigate the dependence of the susceptibility on the interparticle distance as well as on the material parameters of the hybrid system. We find that the susceptibility of the quantum dot exhibits optical transparency for specific frequencies. In addition, we show that there is a range of frequencies of the applied field for which the susceptibility of the semiconductor quantum dot leads to gain. This suggests that in such a hybrid system quantum coherence can reverse the course of energy transfer, allowing flow of energy from the metallic nanoparticle to the quantum dot. We also explore the susceptibility of the metal nanoparticle and show that it is strongly influenced by the presence of the quantum dot.
Wei, Hai-Rui; Lu Long, Gui
2015-01-01
Hybrid quantum gates hold great promise for quantum information processing since they preserve the advantages of different quantum systems. Here we present compact quantum circuits to deterministically implement controlled-NOT, Toffoli, and Fredkin gates between a flying photon qubit and diamond nitrogen-vacancy (NV) centers assisted by microcavities. The target qubits of these universal quantum gates are encoded on the spins of the electrons associated with the diamond NV centers and they have long coherence time for storing information, and the control qubit is encoded on the polarizations of the flying photon and can be easily manipulated. Our quantum circuits are compact, economic, and simple. Moreover, they do not require additional qubits. The complexity of our schemes for universal three-qubit gates is much reduced, compared to the synthesis with two-qubit entangling gates. These schemes have high fidelities and efficiencies, and they are feasible in experiment. PMID:26271899
All-optical quantum computing with a hybrid solid-state processing unit
International Nuclear Information System (INIS)
Pei Pei; Zhang Fengyang; Li Chong; Song Heshan
2011-01-01
We develop an architecture of a hybrid quantum solid-state processing unit for universal quantum computing. The architecture allows distant and nonidentical solid-state qubits in distinct physical systems to interact and work collaboratively. All the quantum computing procedures are controlled by optical methods using classical fields and cavity QED. Our methods have a prominent advantage of the insensitivity to dissipation process benefiting from the virtual excitation of subsystems. Moreover, the quantum nondemolition measurements and state transfer for the solid-state qubits are proposed. The architecture opens promising perspectives for implementing scalable quantum computation in a broader sense that different solid-state systems can merge and be integrated into one quantum processor afterward.
Hybrid Toffoli gate on photons and quantum spins.
Luo, Ming-Xing; Ma, Song-Ya; Chen, Xiu-Bo; Wang, Xiaojun
2015-11-16
Quantum computation offers potential advantages in solving a number of interesting and difficult problems. Several controlled logic gates, the elemental building blocks of quantum computer, have been realized with various physical systems. A general technique was recently proposed that significantly reduces the realization complexity of multiple-control logic gates by harnessing multi-level information carriers. We present implementations of a key quantum circuit: the three-qubit Toffoli gate. By exploring the optical selection rules of one-sided optical microcavities, a Toffoli gate may be realized on all combinations of photon and quantum spins in the QD-cavity. The three general controlled-NOT gates are involved using an auxiliary photon with two degrees of freedom. Our results show that photons and quantum spins may be used alternatively in quantum information processing.
Solving Problem of Graph Isomorphism by Membrane-Quantum Hybrid Model
Directory of Open Access Journals (Sweden)
Artiom Alhazov
2015-10-01
Full Text Available This work presents the application of new parallelization methods based on membrane-quantum hybrid computing to graph isomorphism problem solving. Applied membrane-quantum hybrid computational model was developed by authors. Massive parallelism of unconventional computing is used to implement classic brute force algorithm efficiently. This approach does not suppose any restrictions of considered graphs types. The estimated performance of the model is less then quadratic that makes a very good result for the problem of \\textbf{NP} complexity.
Joint quantum state tomography of an entangled qubit–resonator hybrid
International Nuclear Information System (INIS)
LinPeng, X Y; Zhang, H Z; Xu, K; Li, C Y; Zhong, Y P; Wang, Z L; Wang, H; Xie, Q W
2013-01-01
The integration of superconducting qubits and resonators in one circuit offers a promising solution for quantum information processing (QIP), which also realizes the on-chip analogue of cavity quantum electrodynamics (QED), known as circuit QED. In most prototype circuit designs, qubits are active processing elements and resonators are peripherals. As resonators typically have better coherence performance and more accessible energy levels, it is proposed that the entangled qubit–resonator hybrid can be used as a processing element. To achieve such a goal, an accurate measurement of the hybrid is first necessary. Here we demonstrate a joint quantum state tomography (QST) technique to fully characterize an entangled qubit–resonator hybrid. We benchmarked our QST technique by generating and accurately characterizing multiple states, e.g. |gN〉 + |e(N − 1)〉 where (|g〉 and |e〉) are the ground and excited states of the qubit and (|0〉,…,|N〉) are Fock states of the resonator. We further provided a numerical method to improve the QST efficiency and measured the decoherence dynamics of the bipartite hybrid, witnessing dissipation coming from both the qubit and the N-photon Fock state. As such, the joint QST presents an important step toward actively using the qubit–resonator element for QIP in hybrid quantum devices and for studying circuit QED. (paper)
Geng, Qi; Zhu, Ka-Di
2016-07-10
We have theoretically investigated a hybrid system that is composed of a traditional optomechanical component and an additional charge qubit (Cooper pair box) that induces a new nonlinear interaction. It is shown that the peak in optomechanically induced transparency has been split by the new nonlinear interaction, and the width of the splitting is proportional to the coupling coefficient of this nonlinear interaction. This may give a way to measure the nanomechanical oscillator-qubit coupling coefficient in hybrid quantum systems.
Coherent Dynamics of a Hybrid Quantum Spin-Mechanical Oscillator System
Lee, Kenneth William, III
A fully functional quantum computer must contain at least two important components: a quantum memory for storing and manipulating quantum information and a quantum data bus to securely transfer information between quantum memories. Typically, a quantum memory is composed of a matter system, such as an atom or an electron spin, due to their prolonged quantum coherence. Alternatively, a quantum data bus is typically composed of some propagating degree of freedom, such as a photon, which can retain quantum information over long distances. Therefore, a quantum computer will likely be a hybrid quantum device, consisting of two or more disparate quantum systems. However, there must be a reliable and controllable quantum interface between the memory and bus in order to faithfully interconvert quantum information. The current engineering challenge for quantum computers is scaling the device to large numbers of controllable quantum systems, which will ultimately depend on the choice of the quantum elements and interfaces utilized in the device. In this thesis, we present and characterize a hybrid quantum device comprised of single nitrogen-vacancy (NV) centers embedded in a high quality factor diamond mechanical oscillator. The electron spin of the NV center is a leading candidate for the realization of a quantum memory due to its exceptional quantum coherence times. On the other hand, mechanical oscillators are highly sensitive to a wide variety of external forces, and have the potential to serve as a long-range quantum bus between quantum systems of disparate energy scales. These two elements are interfaced through crystal strain generated by vibrations of the mechanical oscillator. Importantly, a strain interface allows for a scalable architecture, and furthermore, opens the door to integration into a larger quantum network through coupling to an optical interface. There are a few important engineering challenges associated with this device. First, there have been no
Biexciton Auger Recombination Differs in Hybrid and Inorganic Halide Perovskite Quantum Dots.
Eperon, Giles E; Jedlicka, Erin; Ginger, David S
2018-01-04
We use time-resolved photoluminescence measurements to determine the biexciton Auger recombination rate in both hybrid organic-inorganic and fully inorganic halide perovskite nanocrystals as a function of nanocrystal volume. We find that the volume scaling of the biexciton Auger rate in the hybrid perovskites, containing a polar organic A-site cation, is significantly shallower than in the fully inorganic Cs-based nanocrystals. As the nanocrystals become smaller, the Auger rate in the hybrid nanocrystals increases even less than expected, compared to the fully inorganic nanocrystals, which already show a shallower volume dependence than other material systems such as chalcogenide quantum dots. This finding suggests there may be differences in the strength of Coulombic interactions between the fully inorganic and hybrid perovskites, which may prove to be crucial in selecting materials to obtain the highest performing devices in the future, and hints that there could be something "special" about the hybrid materials.
LHCb: Quantum Efficiency of Hybrid Photon Detectors for the LHCb RICH
Lambert, Robert W
2007-01-01
The production of 550 hybrid photon detectors to be used within the LHCb RICH detectors has recently finished. Photonis-DEP have succeeded in consistently improving the tube quantum efficiency, by a relative 27,% with respect to preseries and prototype tubes, when integrated over the energy spectrum.
Tavakoli, Mohammad Mahdi; Tayyebi, Ahmad; Simchi, Abdolreza; Aashuri, Hossein; Outokesh, Mohmmad; Fan, Zhiyong
2015-01-01
Recently, hybrid graphene-quantum dot systems have attracted increasing attention for the next-generation optoelectronic devices such as ultrafast photo-detectors and solar energy harvesting. In this paper, a novel, one-step, reproducible, and solution-processed method is introduced to prepare hybrid graphene-PbS colloids by employing supercritical ethanol. In the hybrid nanocomposite, PbS quantum dots ( 3 nm) are decorated on the reduced graphene oxide (rGO) nanosheets ( 1 nm thickness and less than 1 micron lengths). By employing X-ray photoelectron and Raman and infrared spectroscopy techniques, it is shown that the rGO nanosheets are bonded to PbS nanocrystals through carboxylic bonds. Passivation of {111} planes of PbS quantum dots with rGO nanosheets is demonstrated by employing density function theory. Quenching of the photoluminescence emission of PbS nanocrystals through coupling with graphene sheets is also shown. In order to illustrate that the developed preparation method does not impair the quantum efficiency of the PbS nanocrystals, the photovoltaic efficiency of solar cell device is reported and compared with oleic acid-capped PbS colloidal quantum dot solar cells. By employing the "Hall effect" measurement, it is shown that the carrier mobility is significantly increased (by two orders of magnitudes) in the presence of graphene nanosheets.
Red light emitting solid state hybrid quantum dot-near-UV GaN LED devices
International Nuclear Information System (INIS)
Song, Hongjoo; Lee, Seonghoon
2007-01-01
We produced core-shell (CdSe)ZnSe quantum dots by direct colloidal chemical synthesis and the surface-passivation method-an overcoating of the core CdSe with a larger-bandgap material ZnSe. The (CdSe)ZnSe quantum dots(QDs) play the role of a colour conversion centre. We call these quantum dots nanophosphors. We fabricated red light emitting hybrid devices of (CdSe)ZnSe QDs and a near-UV GaN LED by combining red light emitting (CdSe)ZnSe quantum dots (as a colour conversion centre) with a near-UV(NUV) GaN LED chip (as an excitation source). A few good red phosphors have been known for UV excitation wavelengths, and red phosphors for UV excitation have been sought for a long time. Here we tested the possibility of using (CdSe)ZnSe QDs as red nanophosphors for UV excitation. The fabricated red light emitting hybrid device of (CdSe)ZnSe and a NUV GaN LED chip showed a good luminance. We demonstrated that the (CdSe)ZnSe quantum dots were promising red nanophosphors for NUV excitation and that a red LED made of QDs and a NUV excitation source was a highly efficient hybrid device
Hybrid quantum circuit with a superconducting qubit coupled to an electron spin ensemble
Energy Technology Data Exchange (ETDEWEB)
Kubo, Yuimaru; Grezes, Cecile; Vion, Denis; Esteve, Daniel; Bertet, Patrice [Quantronics Group, SPEC (CNRS URA 2464), CEA-Saclay, 91191 Gif-sur-Yvette (France); Diniz, Igor; Auffeves, Alexia [Institut Neel, CNRS, BP 166, 38042 Grenoble (France); Isoya, Jun-ichi [Research Center for Knowledge Communities, University of Tsukuba, 305-8550 Tsukuba (Japan); Jacques, Vincent; Dreau, Anais; Roch, Jean-Francois [LPQM (CNRS, UMR 8537), Ecole Normale Superieure de Cachan, 94235 Cachan (France)
2013-07-01
We report the experimental realization of a hybrid quantum circuit combining a superconducting qubit and an ensemble of electronic spins. The qubit, of the transmon type, is coherently coupled to the spin ensemble consisting of nitrogen-vacancy (NV) centers in a diamond crystal via a frequency-tunable superconducting resonator acting as a quantum bus. Using this circuit, we prepare arbitrary superpositions of the qubit states that we store into collective excitations of the spin ensemble and retrieve back into the qubit. We also report a new method for detecting the magnetic resonance of electronic spins at low temperature with a qubit using the hybrid quantum circuit, as well as our recent progress on spin echo experiments.
Quantum State Transmission in a Superconducting Charge Qubit-Atom Hybrid
Yu, Deshui; Valado, María Martínez; Hufnagel, Christoph; Kwek, Leong Chuan; Amico, Luigi; Dumke, Rainer
2016-01-01
Hybrids consisting of macroscopic superconducting circuits and microscopic components, such as atoms and spins, have the potential of transmitting an arbitrary state between different quantum species, leading to the prospective of high-speed operation and long-time storage of quantum information. Here we propose a novel hybrid structure, where a neutral-atom qubit directly interfaces with a superconducting charge qubit, to implement the qubit-state transmission. The highly-excited Rydberg atom located inside the gate capacitor strongly affects the behavior of Cooper pairs in the box while the atom in the ground state hardly interferes with the superconducting device. In addition, the DC Stark shift of the atomic states significantly depends on the charge-qubit states. By means of the standard spectroscopic techniques and sweeping the gate voltage bias, we show how to transfer an arbitrary quantum state from the superconducting device to the atom and vice versa. PMID:27922087
Tunneling conductance in superconductor-hybrid double quantum dots Josephson junction
Chamoli, Tanuj; Ajay
2018-05-01
The present work deals with the theoretical model study to analyse the tunneling conductance across a superconductor hybrid double quantum dots tunnel junction (S-DQD-S). Recently, there are many experimental works where the Josephson current across such nanoscopic junction is found to be dependent on nature of the superconducting electrodes, coupling of the hybrid double quantum dot's electronic states with the electronic states of the superconductors and nature of electronic structure of the coupled dots. For this, we have attempted a theoretical model containing contributions of BCS superconducting leads, magnetic coupled quantum dot states and coupling of superconducting leads with QDs. In order to include magnetic coupled QDs the contributions of competitive Kondo and Ruderman-Kittel- Kasuya-Yosida (RKKY) interaction terms are also introduced through many body effects in the model Hamiltonian at low temperatures (where Kondo temperature TK tunnel junctions. Tunneling conductance is proportional to DOS, hence we can analyse it's behaviour with the help of DOS.
International Nuclear Information System (INIS)
Zhao, Dongxing; Wu, Jiarui; Gu, Ying; Gong, Qihuang
2014-01-01
We propose tailoring of the double Fano profiles via plasmon-assisted quantum interference in a hybrid exciton-plasmon system. Tailoring is performed by the interference between two exciton channels interacting with a common localized surface plasmon. Using an applied field of low intensity, the absorption spectrum of the hybrid system reveals a double Fano lineshape with four peaks. For relatively large field intensity, a broad flat window in the absorption spectrum appears which results from the destructive interference between excitons. Because of strong constructive interference, this window vanishes as intensity is further increased. We have designed a nanometer bandpass optical filter for visible light based on tailoring of the optical spectrum. This study provides a platform for quantum interference that may have potential applications in ultracompact tunable quantum devices.
A quantum hybrid with a thin antenna at the vertex of a wedge
Energy Technology Data Exchange (ETDEWEB)
Carlone, Raffaele, E-mail: raffaele.carlone@unina.it [Università “Federico II” di Napoli, Dipartimento di Matematica e Applicazioni “R. Caccioppoli”, MSA, via Cinthia, I-80126, Napoli (Italy); Posilicano, Andrea, E-mail: andrea.posilicano@uninsubria.it [DiSAT, Università dell' Insubria, via Valleggio 11, I-22100, Como (Italy)
2017-03-26
We study the spectrum, resonances and scattering matrix of a quantum Hamiltonian on a “hybrid surface” consisting of a half-line attached by its endpoint to the vertex of a concave planar wedge. At the boundary of the wedge, outside the vertex, homogeneous Dirichlet conditions are imposed. The system is tunable by varying the measure of the angle at the vertex. - Highlights: • Spectral characterization of a quantum Hamiltonian on “hybrid surface” consisting of a halfline attached to the vertex of a concave planar wedge. • The system is tunable by varying the measure of the angle at the vertex. • Relation between the conduction properties inside the hybrid and formation of resonances. • Easy generalization of the results to more complicated structures.
Quantum teleportation and entanglement. A hybrid approach to optical quantum information procesing
Energy Technology Data Exchange (ETDEWEB)
Furusawa, Akira [Tokyo Univ. (Japan). Dept. of Applied Physics; Loock, Peter van [Erlangen-Nuernberg Univ. (Germany). Lehrstuhl fuer Optik
2011-07-01
Unique in that it is jointly written by an experimentalist and a theorist, this monograph presents universal quantum computation based on quantum teleportation as an elementary subroutine and multi-party entanglement as a universal resource. Optical approaches to measurement-based quantum computation are also described, including schemes for quantum error correction, with most of the experiments carried out by the authors themselves. Ranging from the theoretical background to the details of the experimental realization, the book describes results and advances in the field, backed by numerous illustrations of the authors' experimental setups. Aimed at researchers, physicists, and graduate and PhD students in physics, theoretical quantum optics, quantum mechanics, and quantum information. (orig.)
Hybrid threshold adaptable quantum secret sharing scheme with reverse Huffman-Fibonacci-tree coding.
Lai, Hong; Zhang, Jun; Luo, Ming-Xing; Pan, Lei; Pieprzyk, Josef; Xiao, Fuyuan; Orgun, Mehmet A
2016-08-12
With prevalent attacks in communication, sharing a secret between communicating parties is an ongoing challenge. Moreover, it is important to integrate quantum solutions with classical secret sharing schemes with low computational cost for the real world use. This paper proposes a novel hybrid threshold adaptable quantum secret sharing scheme, using an m-bonacci orbital angular momentum (OAM) pump, Lagrange interpolation polynomials, and reverse Huffman-Fibonacci-tree coding. To be exact, we employ entangled states prepared by m-bonacci sequences to detect eavesdropping. Meanwhile, we encode m-bonacci sequences in Lagrange interpolation polynomials to generate the shares of a secret with reverse Huffman-Fibonacci-tree coding. The advantages of the proposed scheme is that it can detect eavesdropping without joint quantum operations, and permits secret sharing for an arbitrary but no less than threshold-value number of classical participants with much lower bandwidth. Also, in comparison with existing quantum secret sharing schemes, it still works when there are dynamic changes, such as the unavailability of some quantum channel, the arrival of new participants and the departure of participants. Finally, we provide security analysis of the new hybrid quantum secret sharing scheme and discuss its useful features for modern applications.
On-chip single photon filtering and multiplexing in hybrid quantum photonic circuits.
Elshaari, Ali W; Zadeh, Iman Esmaeil; Fognini, Andreas; Reimer, Michael E; Dalacu, Dan; Poole, Philip J; Zwiller, Val; Jöns, Klaus D
2017-08-30
Quantum light plays a pivotal role in modern science and future photonic applications. Since the advent of integrated quantum nanophotonics different material platforms based on III-V nanostructures-, colour centers-, and nonlinear waveguides as on-chip light sources have been investigated. Each platform has unique advantages and limitations; however, all implementations face major challenges with filtering of individual quantum states, scalable integration, deterministic multiplexing of selected quantum emitters, and on-chip excitation suppression. Here we overcome all of these challenges with a hybrid and scalable approach, where single III-V quantum emitters are positioned and deterministically integrated in a complementary metal-oxide-semiconductor-compatible photonic circuit. We demonstrate reconfigurable on-chip single-photon filtering and wavelength division multiplexing with a foot print one million times smaller than similar table-top approaches, while offering excitation suppression of more than 95 dB and efficient routing of single photons over a bandwidth of 40 nm. Our work marks an important step to harvest quantum optical technologies' full potential.Combining different integration platforms on the same chip is currently one of the main challenges for quantum technologies. Here, Elshaari et al. show III-V Quantum Dots embedded in nanowires operating in a CMOS compatible circuit, with controlled on-chip filtering and tunable routing.
Optical properties of hybrid quantum-well–dots nanostructures grown by MOCVD
Energy Technology Data Exchange (ETDEWEB)
Mintairov, S. A., E-mail: mintairov@scell.ioffe.ru; Kalyuzhnyy, N. A.; Nadtochiy, A. M.; Maximov, M. V. [St. Petersburg Academic University (Russian Federation); Rouvimov, S. S. [University of Notre Dame (United States); Zhukov, A. E. [St. Petersburg Academic University (Russian Federation)
2017-03-15
The deposition of In{sub x}Ga{sub 1–x}As with an indium content of 0.3–0.5 and an average thickness of 3–27 single layers on a GaAs wafer by metalorganic chemical vapor deposition (MOCVD) at low temperatures results in the appearance of thickness and composition modulations in the layers being formed. Such structures can be considered to be intermediate nanostructures between ideal quantum wells and quantum dots. Depending on the average thickness and composition of the layers, the wavelength of the photoluminescence peak for the hybrid InGaAs quantum well–dots nanostructures varies from 950 to 1100 nm. The optimal average In{sub x}Ga{sub 1–x}As thicknesses and compositions at which the emission wavelength is the longest with a high quantum efficiency retained are determined.
Hybrid zinc oxide/graphene electrodes for depleted heterojunction colloidal quantum-dot solar cells.
Tavakoli, Mohammad Mahdi; Aashuri, Hossein; Simchi, Abdolreza; Fan, Zhiyong
2015-10-07
Recently, hybrid nanocomposites consisting of graphene/nanomaterial heterostructures have emerged as promising candidates for the fabrication of optoelectronic devices. In this work, we have employed a facile and in situ solution-based process to prepare zinc oxide/graphene quantum dots (ZnO/G QDs) in a hybrid structure. The prepared hybrid dots are composed of a ZnO core, with an average size of 5 nm, warped with graphene nanosheets. Spectroscopic studies show that the graphene shell quenches the photoluminescence intensity of the ZnO nanocrystals by about 72%, primarily due to charge transfer reactions and static quenching. A red shift in the absorption peak is also observed. Raman spectroscopy determines G-band splitting of the graphene shell into two separated sub-bands (G(+), G(-)) caused by the strain induced symmetry breaking. It is shown that the hybrid ZnO/G QDs can be used as a counter-electrode for heterojunction colloidal quantum-dot solar cells for efficient charge-carrier collection, as evidenced by the external quantum efficiency measurement. Under the solar simulated spectrum (AM 1.5G), we report enhanced power conversion efficiency (35%) with higher short current circuit (80%) for lead sulfide-based solar cells as compared to devices prepared by pristine ZnO nanocrystals.
Charge Dynamics and Spin Blockade in a Hybrid Double Quantum Dot in Silicon
Directory of Open Access Journals (Sweden)
Matias Urdampilleta
2015-08-01
Full Text Available Electron spin qubits in silicon, whether in quantum dots or in donor atoms, have long been considered attractive qubits for the implementation of a quantum computer because of silicon’s “semiconductor vacuum” character and its compatibility with the microelectronics industry. While donor electron spins in silicon provide extremely long coherence times and access to the nuclear spin via the hyperfine interaction, quantum dots have the complementary advantages of fast electrical operations, tunability, and scalability. Here, we present an approach to a novel hybrid double quantum dot by coupling a donor to a lithographically patterned artificial atom. Using gate-based rf reflectometry, we probe the charge stability of this double quantum-dot system and the variation of quantum capacitance at the interdot charge transition. Using microwave spectroscopy, we find a tunnel coupling of 2.7 GHz and characterize the charge dynamics, which reveals a charge T_{2}^{*} of 200 ps and a relaxation time T_{1} of 100 ns. Additionally, we demonstrate a spin blockade at the inderdot transition, opening up the possibility to operate this coupled system as a singlet-triplet qubit or to transfer a coherent spin state between the quantum dot and the donor electron and nucleus.
Hybrid Integration of Solid-State Quantum Emitters on a Silicon Photonic Chip.
Kim, Je-Hyung; Aghaeimeibodi, Shahriar; Richardson, Christopher J K; Leavitt, Richard P; Englund, Dirk; Waks, Edo
2017-12-13
Scalable quantum photonic systems require efficient single photon sources coupled to integrated photonic devices. Solid-state quantum emitters can generate single photons with high efficiency, while silicon photonic circuits can manipulate them in an integrated device structure. Combining these two material platforms could, therefore, significantly increase the complexity of integrated quantum photonic devices. Here, we demonstrate hybrid integration of solid-state quantum emitters to a silicon photonic device. We develop a pick-and-place technique that can position epitaxially grown InAs/InP quantum dots emitting at telecom wavelengths on a silicon photonic chip deterministically with nanoscale precision. We employ an adiabatic tapering approach to transfer the emission from the quantum dots to the waveguide with high efficiency. We also incorporate an on-chip silicon-photonic beamsplitter to perform a Hanbury-Brown and Twiss measurement. Our approach could enable integration of precharacterized III-V quantum photonic devices into large-scale photonic structures to enable complex devices composed of many emitters and photons.
Strain-mediated coupling in a quantum dot-mechanical oscillator hybrid system.
Yeo, I; de Assis, P-L; Gloppe, A; Dupont-Ferrier, E; Verlot, P; Malik, N S; Dupuy, E; Claudon, J; Gérard, J-M; Auffèves, A; Nogues, G; Seidelin, S; Poizat, J-Ph; Arcizet, O; Richard, M
2014-02-01
Recent progress in nanotechnology has allowed the fabrication of new hybrid systems in which a single two-level system is coupled to a mechanical nanoresonator. In such systems the quantum nature of a macroscopic degree of freedom can be revealed and manipulated. This opens up appealing perspectives for quantum information technologies, and for the exploration of the quantum-classical boundary. Here we present the experimental realization of a monolithic solid-state hybrid system governed by material strain: a quantum dot is embedded within a nanowire that features discrete mechanical resonances corresponding to flexural vibration modes. Mechanical vibrations result in a time-varying strain field that modulates the quantum dot transition energy. This approach simultaneously offers a large light-extraction efficiency and a large exciton-phonon coupling strength g0. By means of optical and mechanical spectroscopy, we find that g0/2 π is nearly as large as the mechanical frequency, a criterion that defines the ultrastrong coupling regime.
Universal quantum gates for photon-atom hybrid systems assisted by bad cavities
Wang, Guan-Yu; Liu, Qian; Wei, Hai-Rui; Li, Tao; Ai, Qing; Deng, Fu-Guo
2016-01-01
We present two deterministic schemes for constructing a CNOT gate and a Toffoli gate on photon-atom and photon-atom-atom hybrid quantum systems assisted by bad cavities, respectively. They are achieved by cavity-assisted photon scattering and work in the intermediate coupling region with bad cavities, which relaxes the difficulty of their implementation in experiment. Also, bad cavities are feasible for fast quantum operations and reading out information. Compared with previous works, our schemes do not need any auxiliary qubits and measurements. Moreover, the schematic setups for these gates are simple, especially that for our Toffoli gate as only a quarter wave packet is used to interact the photon with each of the atoms every time. These atom-cavity systems can be used as the quantum nodes in long-distance quantum communication as their relatively long coherence time is suitable for multi-time operations between the photon and the system. Our calculations show that the average fidelities and efficiencies of our two universal hybrid quantum gates are high with current experimental technology. PMID:27067992
Energy Technology Data Exchange (ETDEWEB)
Bubanja, Vladimir, E-mail: vladimir.bubanja@callaghaninnovation.govt.nz
2015-06-15
We present schemes for quantum teleportation and entanglement swapping of electronic spin states in hybrid superconductor–normal-metal systems. The proposed schemes employ subgap transport whereby the lowest order processes involve Cooper pair-electron and double Cooper-pair cotunneling in quantum teleportation and entanglement swapping protocols, respectively. The competition between elastic cotunneling and Cooper-pair splitting results in the success probability of 25% in both cases. Described implementations of these protocols are within reach of present-day experimental techniques.
Application of Hybrid Quantum Tabu Search with Support Vector Regression (SVR for Load Forecasting
Directory of Open Access Journals (Sweden)
Cheng-Wen Lee
2016-10-01
Full Text Available Hybridizing chaotic evolutionary algorithms with support vector regression (SVR to improve forecasting accuracy is a hot topic in electricity load forecasting. Trapping at local optima and premature convergence are critical shortcomings of the tabu search (TS algorithm. This paper investigates potential improvements of the TS algorithm by applying quantum computing mechanics to enhance the search information sharing mechanism (tabu memory to improve the forecasting accuracy. This article presents an SVR-based load forecasting model that integrates quantum behaviors and the TS algorithm with the support vector regression model (namely SVRQTS to obtain a more satisfactory forecasting accuracy. Numerical examples demonstrate that the proposed model outperforms the alternatives.
Functionalized Self-Assembled InAs/GaAs Quantum-Dot Structures Hybridized with Organic Molecules
DEFF Research Database (Denmark)
Chen, Miaoxiang Max; Kobashi, K.; Chen, B.
2010-01-01
Low-dimensional III-V semiconductors have many advantages over other semiconductors; however, they are not particularly stable under physiological conditions. Hybridizing biocompatible organic molecules with advanced optical and electronic semiconductor devices based on quantum dots (QDs...
Nair, Lakshmi V; Nagaoka, Yutaka; Maekawa, Toru; Sakthikumar, D; Jayasree, Ramapurath S
2014-07-23
Hybrid nanomaterial based on quantum dots and SWCNTs is used for cellular imaging and photothermal therapy. Furthermore, the ligand conjugated hybrid system (FaQd@CNT) enables selective targeting in cancer cells. The imaging capability of quantum dots and the therapeutic potential of SWCNT are available in a single system with cancer targeting property. Heat generated by the system is found to be high enough to destroy cancer cells. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Quantum transport in nanowire-based hybrid devices
Energy Technology Data Exchange (ETDEWEB)
Guenel, Haci Yusuf
2013-05-08
We have studied the low-temperature transport properties of nanowires contacted by a normal metal as well as by superconducting electrodes. As a consequence of quantum coherence, we have demonstrated the electron interference effect in different aspects. The mesoscopic phase coherent transport properties were studied by contacting the semiconductor InAs and InSb nanowires with normal metal electrodes. Moreover, we explored the interaction of the microscopic quantum coherence of the nanowires with the macroscopic quantum coherence of the superconductors. In superconducting Nb contacted InAs nanowire junctions, we have investigated the effect of temperature, magnetic field and electric field on the supercurrent. Owing to relatively high critical temperature of superconducting Nb (T{sub c} ∝ 9 K), we have observed the supercurrent up to 4 K for highly doped nanowire-based junctions, while for low doped nanowire-based junctions a full control of the supercurrent was achieved. Due to low transversal dimension of the nanowires, we have found a monotonous decay of the critical current in magnetic field dependent measurements. The experimental results were analyzed within narrow junction model which has been developed recently. At high bias voltages, we have observed subharmonic energy gap structures as a consequence of multiple Andreev reflection. Some of the nanowires were etched, such that the superconducting Nb electrodes are connected to both ends of the nanowire rather than covering the surface of the nanowire. As a result of well defined nanowire-superconductor interfaces, we have examined quasiparticle interference effect in magnetotransport measurements. Furthermore, we have developed a new junction geometry, such that one of the superconducting Nb electrodes is replaced by a superconducting Al. Owing to the smaller critical magnetic field of superconducting Al (B{sub c} ∝ 15-50,mT), compared to superconducting Nb (B{sub c} ∝ 3 T), we were able to studied
Hybrid magic state distillation for universal fault-tolerant quantum computation
Zheng, Wenqiang; Yu, Yafei; Pan, Jian; Zhang, Jingfu; Li, Jun; Li, Zhaokai; Suter, Dieter; Zhou, Xianyi; Peng, Xinhua; Du, Jiangfeng
2014-01-01
A set of stabilizer operations augmented by some special initial states known as 'magic states', gives the possibility of universal fault-tolerant quantum computation. However, magic state preparation inevitably involves nonideal operations that introduce noise. The most common method to eliminate the noise is magic state distillation (MSD) by stabilizer operations. Here we propose a hybrid MSD protocol by connecting a four-qubit H-type MSD with a five-qubit T-type MSD, in order to overcome s...
Hybrid ququart-encoded quantum cryptography protected by Kochen-Specker contextuality
International Nuclear Information System (INIS)
Cabello, Adan; D'Ambrosio, Vincenzo; Nagali, Eleonora; Sciarrino, Fabio
2011-01-01
Quantum cryptographic protocols based on complementarity are not secure against attacks in which complementarity is imitated with classical resources. The Kochen-Specker (KS) theorem provides protection against these attacks, without requiring entanglement or spatially separated composite systems. We analyze the maximum tolerated noise to guarantee the security of a KS-protected cryptographic scheme against these attacks and describe a photonic realization of this scheme using hybrid ququarts defined by the polarization and orbital angular momentum of single photons.
An alternative route towards monodisperse CdS quantum dots for hybrid solar cells
International Nuclear Information System (INIS)
Cao, Fengfeng; Wang, Hao; Xia, Zhouhui; Dai, Xiao; Cong, Shan; Dong, Chao; Sun, Baoquan; Lou, Yanhui; Sun, Yinghui; Zhao, Jie; Zou, Guifu
2015-01-01
Monodisperse CdS quantum dots (QDs) are synthesized by thermal decomposition of organic complexes in the system of the cost-effective commercial 0 # diesel at 200 °C. The prepared CdS QDs have a good dispersion and high crystallization. When the CdS QDs are doped into the blends of poly(3-hexylthiophene) (P3HT) and 1-(3-methoxycarbonyl)-propyl-1-phenyl-(6, 6)C61 (PCBM) for hybrid solar cells (HSCs), the HSCs achieve about 25% increase of power conversion efficiency in comparison to the reference device without the CdS QDs. The improvement of the cell performance mainly attributes to the increased short-circuit current density arising from the absorption enhancement in the wavelength range of 350–550 nm by introducing the synthesized CdS QDs into the P3HT: PCBM active layer. - Highlights: • Monodisperse CdS quantum dots. • A cost-effective route to synthesize crystalline CdS quantum dots. • CdS quantum dots based hybrid solar cells with power conversion efficiency enhancement
An alternative route towards monodisperse CdS quantum dots for hybrid solar cells
Energy Technology Data Exchange (ETDEWEB)
Cao, Fengfeng; Wang, Hao [College of Physics, Optoelectronics and Energy and Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006 (China); Xia, Zhouhui [Institute of Functional Nano and Soft Materials, Soochow University, Suzhou 215123 (China); Dai, Xiao; Cong, Shan [College of Physics, Optoelectronics and Energy and Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006 (China); Dong, Chao [Department of Chemistry and Biology, University of New Mexico, ABQ 87120 (United States); Sun, Baoquan [Institute of Functional Nano and Soft Materials, Soochow University, Suzhou 215123 (China); Lou, Yanhui, E-mail: yhlou@suda.edu.cn [College of Physics, Optoelectronics and Energy and Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006 (China); Sun, Yinghui; Zhao, Jie [College of Physics, Optoelectronics and Energy and Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006 (China); Zou, Guifu, E-mail: zouguifu@suda.edu.cn [College of Physics, Optoelectronics and Energy and Collaborative Innovation Center of Suzhou Nano Science and Technology, Soochow University, Suzhou 215006 (China)
2015-01-15
Monodisperse CdS quantum dots (QDs) are synthesized by thermal decomposition of organic complexes in the system of the cost-effective commercial 0{sup #} diesel at 200 °C. The prepared CdS QDs have a good dispersion and high crystallization. When the CdS QDs are doped into the blends of poly(3-hexylthiophene) (P3HT) and 1-(3-methoxycarbonyl)-propyl-1-phenyl-(6, 6)C61 (PCBM) for hybrid solar cells (HSCs), the HSCs achieve about 25% increase of power conversion efficiency in comparison to the reference device without the CdS QDs. The improvement of the cell performance mainly attributes to the increased short-circuit current density arising from the absorption enhancement in the wavelength range of 350–550 nm by introducing the synthesized CdS QDs into the P3HT: PCBM active layer. - Highlights: • Monodisperse CdS quantum dots. • A cost-effective route to synthesize crystalline CdS quantum dots. • CdS quantum dots based hybrid solar cells with power conversion efficiency enhancement.
Biocompatible Polymer/Quantum Dots Hybrid Materials: Current Status and Future Developments
Directory of Open Access Journals (Sweden)
Lei Shen
2011-12-01
Full Text Available Quantum dots (QDs are nanometer-sized semiconductor particles with tunable fluorescent optical property that can be adjusted by their chemical composition, size, or shape. In the past 10 years, they have been demonstrated as a powerful fluorescence tool for biological and biomedical applications, such as diagnostics, biosensing and biolabeling. QDs with high fluorescence quantum yield and optical stability are usually synthesized in organic solvents. In aqueous solution, however, their metallic toxicity, non-dissolubility and photo-luminescence instability prevent the direct utility of QDs in biological media. Polymers are widely used to cover and coat QDs for fabricating biocompatible QDs. Such hybrid materials can provide solubility and robust colloidal and optical stability in water. At the same time, polymers can carry ionic or reactive functional groups for incorporation into the end-use application of QDs, such as receptor targeting and cell attachment. This review provides an overview of the recent development of methods for generating biocompatible polymer/QDs hybrid materials with desirable properties. Polymers with different architectures, such as homo- and co-polymer, hyperbranched polymer, and polymeric nanogel, have been used to anchor and protect QDs. The resulted biocompatible polymer/QDs hybrid materials show successful applications in the fields of bioimaging and biosensing. While considerable progress has been made in the design of biocompatible polymer/QDs materials, the research challenges and future developments in this area should affect the technologies of biomaterials and biosensors and result in even better biocompatible polymer/QDs hybrid materials.
Directory of Open Access Journals (Sweden)
Pietra Paola
2012-04-01
Full Text Available We propose a hybrid classical-quantum model to study the motion of electrons in ultra-scaled confined nanostructures. The transport of charged particles, considered as one dimensional, is described by a quantum effective mass model in the active zone coupled directly to a drift-diffusion problem in the rest of the device. We explain how this hybrid model takes into account the peculiarities due to the strong confinement and we present numerical simulations for a simplified carbon nanotube. Nous proposons un modèle hybride classique-quantique pour décrire le mouvement des électrons dans des nanostructures très fortement confinées. Le transport des particules, consideré unidimensionel, est décrit par un modèle quantique avec masse effective dans la zone active couplé à un problème de dérive-diffusion dans le reste du domaine. Nous expliquons comment ce modèle hybride prend en compte les spécificités de ce très fort confinement et nous présentons des résultats numériques pour un nanotube de carbone simplifié.
Kim, Taesoo
2015-10-01
We investigate hybrid tandem solar cells that rely on the combination of solution-processed depleted-heterojunction colloidal quantum dot (CQD) and bulk heterojunction polymer:fullerene subcells. The hybrid tandem solar cell is monolithically integrated and electrically connected in series with a suitable p-n recombination layer that includes metal oxides and a conjugated polyelectrolyte. We discuss the monolithic integration of the subcells, taking into account solvent interactions with underlayers and associated constraints on the tandem architecture, and show that an adequate device configuration consists of a low bandgap CQD bottom cell and a high bandgap polymer:fullerene top cell. Once we optimize the recombination layer and individual subcells, the hybrid tandem device reaches a VOC of 1.3V, approaching the sum of the individual subcell voltages. An impressive fill factor of 70% is achieved, further confirming that the subcells are efficiently connected via an appropriate recombination layer. © 2015.
Theory of Quantum Transport in Metallic and Hybrid Nanostructures
Glatz, Andreas; Vinokur, Valerii M
2006-01-01
There is a major development emerging at the intersection of modern physics, computer science, and materials science, which struggles to squeeze more devices into a restricted volume and constitutes a central focus of modern nanotechnology. Utilizing the metal-based hybrid nanostructures may offer significant advantages over those exploiting purely semiconductor materials. First, the chemistry of metals is typically simpler than that of semiconductors. Second, the electric properties of metals are much less sensitive to the structural defects and impurities than those of semiconductors. Next, metallic devices allow better electric and thermal contacts. And, last but by no means least, the high electron velocity in metals promises to accelerate enormously operation rates with respect to those in semiconductor-based devices. The book reflects scientific developments in the physics of metallic compounds based nanodevices presented at the NATO-sponsored Workshop on nanophysics held in St. Petersburg, Russia in th...
Hybrid quantum logic and a test of Bell's inequality using two different atomic isotopes.
Ballance, C J; Schäfer, V M; Home, J P; Szwer, D J; Webster, S C; Allcock, D T C; Linke, N M; Harty, T P; Aude Craik, D P L; Stacey, D N; Steane, A M; Lucas, D M
2015-12-17
Entanglement is one of the most fundamental properties of quantum mechanics, and is the key resource for quantum information processing (QIP). Bipartite entangled states of identical particles have been generated and studied in several experiments, and post-selected or heralded entangled states involving pairs of photons, single photons and single atoms, or different nuclei in the solid state, have also been produced. Here we use a deterministic quantum logic gate to generate a 'hybrid' entangled state of two trapped-ion qubits held in different isotopes of calcium, perform full tomography of the state produced, and make a test of Bell's inequality with non-identical atoms. We use a laser-driven two-qubit gate, whose mechanism is insensitive to the qubits' energy splittings, to produce a maximally entangled state of one (40)Ca(+) qubit and one (43)Ca(+) qubit, held 3.5 micrometres apart in the same ion trap, with 99.8 ± 0.6 per cent fidelity. We test the CHSH (Clauser-Horne-Shimony-Holt) version of Bell's inequality for this novel entangled state and find that it is violated by 15 standard deviations; in this test, we close the detection loophole but not the locality loophole. Mixed-species quantum logic is a powerful technique for the construction of a quantum computer based on trapped ions, as it allows protection of memory qubits while other qubits undergo logic operations or are used as photonic interfaces to other processing units. The entangling gate mechanism used here can also be applied to qubits stored in different atomic elements; this would allow both memory and logic gate errors caused by photon scattering to be reduced below the levels required for fault-tolerant quantum error correction, which is an essential prerequisite for general-purpose quantum computing.
Li, Ying
2016-09-16
Fault-tolerant quantum computing in systems composed of both Majorana fermions and topologically unprotected quantum systems, e.g., superconducting circuits or quantum dots, is studied in this Letter. Errors caused by topologically unprotected quantum systems need to be corrected with error-correction schemes, for instance, the surface code. We find that the error-correction performance of such a hybrid topological quantum computer is not superior to a normal quantum computer unless the topological charge of Majorana fermions is insusceptible to noise. If errors changing the topological charge are rare, the fault-tolerance threshold is much higher than the threshold of a normal quantum computer and a surface-code logical qubit could be encoded in only tens of topological qubits instead of about 1,000 normal qubits.
Charge-transfer channel in quantum dot-graphene hybrid materials
Cao, Shuo; Wang, Jingang; Ma, Fengcai; Sun, Mengtao
2018-04-01
The energy band theory of a classical semiconductor can qualitatively explain the charge-transfer process in low-dimensional hybrid colloidal quantum dot (QD)-graphene (GR) materials; however, the definite charge-transfer channels are not clear. Using density functional theory (DFT) and time-dependent DFT, we simulate the hybrid QD-GR nanostructure, and by constructing its orbital interaction diagram, we show the quantitative coupling characteristics of the molecular orbitals (MOs) of the hybrid structure. The main MOs are derived from the fragment MOs (FOs) of GR, and the Cd13Se13 QD FOs merge with the GR FOs in a certain proportion to afford the hybrid system. Upon photoexcitation, electrons in the GR FOs jump to the QD FOs, leaving holes in the GR FOs, and the definite charge-transfer channels can be found by analyzing the complex MOs coupling. The excited electrons and remaining holes can also be localized in the GR or the QD or transfer between the QD and GR with different absorption energies. The charge-transfer process for the selected excited states of the hybrid QD-GR structure are testified by the charge difference density isosurface. The natural transition orbitals, charge-transfer length analysis and 2D site representation of the transition density matrix also verify the electron-hole delocalization, localization, or coherence chacracteristics of the selected excited states. Therefore, our research enhances understanding of the coupling mechanism of low-dimensional hybrid materials and will aid in the design and manipulation of hybrid photoelectric devices for practical application in many fields.
Improved performance of colloidal CdSe quantum dot-sensitized solar cells by hybrid passivation.
Huang, Jing; Xu, Bo; Yuan, Chunze; Chen, Hong; Sun, Junliang; Sun, Licheng; Agren, Hans
2014-11-12
A hybrid passivation strategy is employed to modify the surface of colloidal CdSe quantum dots (QDs) for quantum dot-sensitized solar cells (QDSCs), by using mercaptopropionic acid (MPA) and iodide anions through a ligand exchange reaction in solution. This is found to be an effective way to improve the performance of QDSCs based on colloidal QDs. The results show that MPA can increase the coverage of the QDs on TiO2 electrodes and facilitate the hole extraction from the photoxidized QDs, and simultaneously, that the iodide anions can remedy the surface defects of the CdSe QDs and thus reduce the recombination loss in the device. This hybrid passivation treatment leads to a significant enhancement of the power conversion efficiency of the QDSCs by 41%. Furthermore, an optimal ratio of iodide ions to MPA was determined for favorable hybrid passivation; results show that excessive iodine anions are detrimental to the loading of the QDs. This study demonstrates that the improvement in QDSC performance can be realized by using a combination of different functional ligands to passivate the QDs, and that ligand exchange in solution can be an effective approach to introduce different ligands.
Lee, Ho Won; Lee, Ki-Heon; Lee, Jae Woo; Kim, Jong-Hoon; Yang, Heesun; Kim, Young Kwan
2015-02-01
In this work, the simple process of hybrid quantum dot (QD)/organic light-emitting diode (OLED) was proposed to apply a white illumination light by using QD plate and organic fluorescence. Conventional blue fluorescent OLEDs were firstly fabricated and then QD plates of various concentrations, which can be controlled of UV-vis absorption and photoluminescence spectrum, were attached under glass substrate of completed blue devices. The suggested process indicates that we could fabricate the white device through very simple process without any deposition of orange or red organic emitters. Therefore, this work would be demonstrated that the potential simple process for white applications can be applied and also can be extended to additional research on light applications.
Ramanan, Rajeev; Dubey, Kshatresh Dutta; Wang, Binju; Mandal, Debasish; Shaik, Sason
2016-06-01
This work uses combined quantum mechanical/molecular mechanical and molecular dynamics simulations to investigate the mechanism and selectivity of H2O2-dependent hydroxylation of fatty acids by the P450SPα class of enzymes. H2O2 is found to serve as the surrogate oxidant for generating the principal oxidant, Compound I (Cpd I), in a mechanism that involves homolytic O-O bond cleavage followed by H-abstraction from the Fe-OH moiety. Our results rule out a substrate-assisted heterolytic cleavage of H2O2 en route to Cpd I. We show, however, that substrate binding stabilizes the resultant Fe-H2O2 complex, which is crucial for the formation of Cpd I in the homolytic pathway. A network of hydrogen bonds locks the HO· radical, formed by the O-O homolysis, thus directing it to exclusively abstract the hydrogen atom from Fe-OH, thereby forming Cpd I, while preventing the autoxoidative reaction, with the porphyrin ligand, and the substrate oxidation. The so formed Cpd I subsequently hydroxylates fatty acids at their α-position with S-enantioselectivity. These selectivity patterns are controlled by the active site: substrate's binding by Arg241 determines the α-regioselectivity, while the Pro242 residue locks the prochiral α-CH2, thereby leading to hydroxylation of the pro-S C-H bond. Our study of the mutant Pro242Ala sheds light on potential modifications of the enzyme's active site in order to modify reaction selectivity. Comparisons of P450SPα to P450BM3 and to P450BSβ reveal that function has evolved in these related metalloenzymes by strategically placing very few residues in the active site.
Development of a System for Absolute Quantum Efficiency Determination of Hybrid Photo Diodes
Hammarstedt, P
2001-01-01
At CERN, the European Laboratory for Particle Physics, a new particle accelerator, the Large Hadron Collider (LHC), is under development. The detectors at LHC require development of highly sophisticated technologies, including Hybrid Photo Diodes (HPD) for high efficiency, high resolution single photon detection with a large area coverage. During the HPD development phase, one of the crucial parameters in the optimization of the photocathode creation process is the quantum efficiency. The aim of this Master Thesis has been to design and implement a system for high precision, high resolution quantum efficiency determination over a large, 200-700 nm photon wavelength range. Commercially available components have been obtained, an optomechanical system has been designed and built, and all the necessary data acquisition, control and analysis software has been implemented. The relative precision of the measurement system has been determined to 2%, with additional possible systematic errors less than 2%. Various qu...
Nonequilibrium Quantum Phase Transition in a Hybrid Atom-Optomechanical System
Mann, Niklas; Bakhtiari, M. Reza; Pelster, Axel; Thorwart, Michael
2018-02-01
We consider a hybrid quantum many-body system formed by a vibrational mode of a nanomembrane, which interacts optomechanically with light in a cavity, and an ultracold atom gas in the optical lattice of the out-coupled light. The adiabatic elimination of the light field yields an effective Hamiltonian which reveals a competition between the force localizing the atoms and the membrane displacement. At a critical atom-membrane interaction, we find a nonequilibrium quantum phase transition from a localized symmetric state of the atom cloud to a shifted symmetry-broken state, the energy of the lowest collective excitation vanishes, and a strong atom-membrane entanglement arises. The effect occurs when the atoms and the membrane are nonresonantly coupled.
DEFF Research Database (Denmark)
Hensel, V.; Godt, A.; Popovitz-Biro, R.
2002-01-01
Composite materials of quantum particles (Q-particles) arranged in layers within crystalline powders of pi-conjugated, rodlike dicarboxylic acids are reported. The synthesis of the composites, either as three-dimensional crystals or as thin films at the air-water interface, comprises a two...... analysis of the solids and grazing incidence X-ray diffraction analysis of the films on water. 2) Topotactic solid/gas reaction of these salts with H2S to convert the metal ions into Q-particles of CdS or PbS embedded in the organic matrix that consists of the acids 6(H) and 8(H). These hybrid materials...
Hybrid single quantum well InP/Si nanobeam lasers for silicon photonics.
Fegadolli, William S; Kim, Se-Heon; Postigo, Pablo Aitor; Scherer, Axel
2013-11-15
We report on a hybrid InP/Si photonic crystal nanobeam laser emitting at 1578 nm with a low threshold power of ~14.7 μW. Laser gain is provided from a single InAsP quantum well embedded in a 155 nm InP layer bonded on a standard silicon-on-insulator wafer. This miniaturized nanolaser, with an extremely small modal volume of 0.375(λ/n)(3), is a promising and efficient light source for silicon photonics.
Nayfeh, O. M.; Chao, D.; Djapic, N.; Sims, P.; Liu, B.; Sharma, S.; Lerum, L.; Fahem, M.; Dinh, V.; Zlatanovic, S.; Lynn, B.; Torres, C.; Higa, B.; Moore, J.; Upchurch, A.; Cothern, J.; Tukeman, M.; Barua, R.; Davidson, B.; Ramirez, A. D.; Rees, C. D.; Anant, V.; Kanter, G. S.
2017-08-01
Optically active rare-earth Neodymium (Nd) ions are integrated in Niobium (Nb) thin films forming a new quantum memory device (Nd:Nb) targeting long-lived coherence times and multi-functionality enabled by both spin and photon storage properties. Nb is implanted with Nd spanning 10-60 keV energy and 1013-1014 cm-2 dose producing a 1- 3% Nd:Nb concentration as confirmed by energy-dispersive X-ray spectroscopy. Scanning confocal photoluminescence (PL) at 785 nm excitation are made and sharp emission peaks from the 4F3/2 -red shift and increased broadening to a 4.8 nm linewidth. Nd:Nb is photoconductive and responds strongly to applied fields. Furthermore, optically detected magnetic resonance (ODMR) measurements are presented spanning near-infrared telecom band. The modulation of the emission intensity with magnetic field and microwave power by integration of these magnetic Kramer type Nd ions is quantified along with spin echoes under pulsed microwave π-π/2 excitation. A hybrid system architecture is proposed using spin and photon quantum information storage with the nuclear and electron states of the Nd3+ and neighboring Nb atoms that can couple qubit states to hyperfine 7/2 spin states of Nd:Nb and onto NIR optical levels excitable with entangled single photons, thus enabling implementation of computing and networking/internet protocols in a single platform.
High-response hybrid quantum dots- 2D conductor phototransistors: recent progress and perspectives
Sablon, Kimberly A.; Sergeev, Andrei; Najmaei, Sina; Dubey, Madan
2017-03-01
Having been inspired by the tremendous progress in material nanoscience and device nanoengineering, hybrid phototransistors combine solution processed colloidal semiconductor quantum dots (QDs) with graphene or two-dimensional (2D) semiconductor materials. Novel detectors demonstrate ultrahigh photoconductive gain, high and selective photoresponse, low noise, and very high responsivity in visible- and near-infrared ranges. The outstanding performance of phototransistors is primarily due to the strong, selective, and size tunable absorption of QDs and fast charge transfer in 2D high mobility conductors. However, the relatively small mobility of QD nanomaterials was a technological barrier, which limited the operating rate of devices. Very recent innovations in detector design and significant progress in QD ligand engineering provide effective tools for further qualitative improvements. This article reviews the recent progress in material science, nanophysics, and device engineering related to hybrid phototransistors. Detectors based on various QD nanomaterials and several 2D conductors are compared, and advantages and disadvantages of various nanomaterials for applications in hybrid phototransistors are identified. We also benchmark the experimental characteristics with model results that establish interrelations and tradeoffs between detector characteristics, such as responsivity, dark and noise currents, the photocarrier lifetime, response, and noise bandwidths. We have shown that the most recent phototransistors demonstrate performance limited by the fundamental generation recombination noise in high gain devices. Interrelation between the dynamic range of the detector and the detector sensitivity is discussed. The review is concluded with a brief discussion of the remaining challenges and possible significant improvements in the performance of hybrid phototransistors.
Hybrid tandem quantum dot/organic photovoltaic cells with complementary near infrared absorption
Kim, Taesoo
2017-06-01
Monolithically integrated hybrid tandem solar cells that effectively combine solution-processed colloidal quantum dot (CQD) and organic bulk heterojunction subcells to achieve tandem performance that surpasses the individual subcell efficiencies have not been demonstrated to date. In this work, we demonstrate hybrid tandem cells with a low bandgap PbS CQD subcell harvesting the visible and near-infrared photons and a polymer:fullerene—poly (diketopyrrolopyrrole-terthiophene) (PDPP3T):[6,6]-phenyl-C60-butyric acid methyl ester (PC61BM)—top cell absorbing effectively the red and near-infrared photons of the solar spectrum in a complementary fashion. The two subcells are connected in series via an interconnecting layer (ICL) composed of a metal oxide layer, a conjugated polyelectrolyte, and an ultrathin layer of Au. The ultrathin layer of Au forms nano-islands in the ICL, reducing the series resistance, increasing the shunt resistance, and enhancing the device fill-factor. The hybrid tandems reach a power conversion efficiency (PCE) of 7.9%, significantly higher than the PCE of the corresponding individual single cells, representing one of the highest efficiencies reported to date for hybrid tandem solar cells based on CQD and polymer subcells.
Fabrication of genetically engineered polypeptide@quantum dots hybrid nanogels for targeted imaging
Yang, Jie; Yao, Ming-Hao; Zhao, Dong-Hui; Zhang, Xiao-Shuai; Jin, Rui-Mei; Zhao, Yuan-Di; Liu, Bo
2017-08-01
Nanogels have been widely used as multifunctional drug delivery carriers because of high water content, biocompatibility, and high loading capability. We designed and biosynthesized two triblock artificial polypeptides PC10A and PC10ARGD as vehicles for encapsulating hydrophobic materials. These polypeptides can form nanogels by self-assembly when the concentration is below 2% ( w/ v). The physical properties of nanogels, including size, surface potential, and targeting domain, are able to be tuned. Hydrophobic materials from molecular size to nano-size can be loaded into the polypeptide nanogels to form hybrid nanogels. Hydrophobic quantum dots CdSe@ZnS below 10 nM were loaded into the polypeptide nanogels by ultrasonic treatment. Encapsulation endows hydrophobic QDs with good tunability of size, water solubility, stability, targeting, and biocompatibility. PC10ARGD nanogels and PC10ARGD@QDs hybrid nanogels showed excellent biocompatibility, which the cellular viabilities of HeLa and MCF-7 cells treated with 1% PC10ARGD nanogels and PC10ARGD@QDs hybrid nanogels contained 20 nM QDs were above 90 and 80%, respectively. PC10ARGD@QDs hybrid nanogels with an arginine-glycine-aspartic acid motif present efficient receptor-mediated endocytosis in α v β 3 overexpressing HeLa cells but not in the control MCF-7 cells as analyzed by confocal microscopy. These results demonstrate that such polypeptide nanogels as nanocarriers are expected to have great potential applications in biomedicine.
Directory of Open Access Journals (Sweden)
Kurochkina M
2018-04-01
Full Text Available Margarita Kurochkina,1 Elena Konshina,1 Aleksandr Oseev,2 Soeren Hirsch3 1Centre of Information Optical Technologies, ITMO University, Saint Petersburg, Russia; 2Institute of Micro and Sensor Systems, Otto-von-Guericke-University Magdeburg, Magdeburg, Germany; 3Department of Engineering, University of Applied Sciences Brandenburg, Brandenburg an der Havel, Germany Background: The luminescence amplification of semiconductor quantum dots (QD in the presence of self-assembled gold nanoparticles (Au NPs is one of way for creating biosensors with highly efficient transduction. Aims: The objective of this study was to fabricate the hybrid structures based on semiconductor CdSe/ZnS QDs and Au NP arrays and to use them as biosensors of protein. Methods: In this paper, the hybrid structures based on CdSe/ZnS QDs and Au NP arrays were fabricated using spin coating processes. Au NP arrays deposited on a glass wafer were investigated by optical microscopy and absorption spectroscopy depending on numbers of spin coating layers and their baking temperature. Bovine serum albumin (BSA was used as the target protein analyte in a phosphate buffer. A confocal laser scanning microscope was used to study the luminescent properties of Au NP/QD hybrid structures and to test BSA. Results: The dimensions of Au NP aggregates increased and the space between them decreased with increasing processing temperature. At the same time, a blue shift of the plasmon resonance peak in the absorption spectra of Au NP arrays was observed. The deposition of CdSe/ZnS QDs with a core diameter of 5 nm on the surface of the Au NP arrays caused an increase in absorption and a red shift of the plasmon peak in the spectra. The exciton–plasmon enhancement of the QDs’ photoluminescence intensity has been obtained at room temperature for hybrid structures with Au NPs array pretreated at temperatures of 100°C and 150°C. It has been found that an increase in the weight content of BSA
Wang, Guanglei; Xu, Hongya; Lai, Ying-Cheng
2018-03-01
We present a novel class of nonlinear dynamical systems-a hybrid of relativistic quantum and classical systems and demonstrate that multistability is ubiquitous. A representative setting is coupled systems of a topological insulator and an insulating ferromagnet, where the former possesses an insulating bulk with topologically protected, dissipationless, and conducting surface electronic states governed by the relativistic quantum Dirac Hamiltonian and the latter is described by the nonlinear classical evolution of its magnetization vector. The interactions between the two are essentially the spin transfer torque from the topological insulator to the ferromagnet and the local proximity induced exchange coupling in the opposite direction. The hybrid system exhibits a rich variety of nonlinear dynamical phenomena besides multistability such as bifurcations, chaos, and phase synchronization. The degree of multistability can be controlled by an external voltage. In the case of two coexisting states, the system is effectively binary, opening a door to exploitation for developing spintronic memory devices. Because of the dissipationless and spin-momentum locking nature of the surface currents of the topological insulator, little power is needed for generating a significant current, making the system appealing for potential applications in next generation of low power memory devices.
Hybridizing DEMD and Quantum PSO with SVR in Electric Load Forecasting
Directory of Open Access Journals (Sweden)
Li-Ling Peng
2016-03-01
Full Text Available Electric load forecasting is an important issue for a power utility, associated with the management of daily operations such as energy transfer scheduling, unit commitment, and load dispatch. Inspired by strong non-linear learning capability of support vector regression (SVR, this paper presents an SVR model hybridized with the differential empirical mode decomposition (DEMD method and quantum particle swarm optimization algorithm (QPSO for electric load forecasting. The DEMD method is employed to decompose the electric load to several detail parts associated with high frequencies (intrinsic mode function—IMF and an approximate part associated with low frequencies. Hybridized with quantum theory to enhance particle searching performance, the so-called QPSO is used to optimize the parameters of SVR. The electric load data of the New South Wales (Sydney, Australia market and the New York Independent System Operator (NYISO, New York, USA are used for comparing the forecasting performances of different forecasting models. The results illustrate the validity of the idea that the proposed model can simultaneously provide forecasting with good accuracy and interpretability.
Emergence, evolution, and control of multistability in a hybrid topological quantum/classical system
Wang, Guanglei; Xu, Hongya; Lai, Ying-Cheng
2018-03-01
We present a novel class of nonlinear dynamical systems—a hybrid of relativistic quantum and classical systems and demonstrate that multistability is ubiquitous. A representative setting is coupled systems of a topological insulator and an insulating ferromagnet, where the former possesses an insulating bulk with topologically protected, dissipationless, and conducting surface electronic states governed by the relativistic quantum Dirac Hamiltonian and the latter is described by the nonlinear classical evolution of its magnetization vector. The interactions between the two are essentially the spin transfer torque from the topological insulator to the ferromagnet and the local proximity induced exchange coupling in the opposite direction. The hybrid system exhibits a rich variety of nonlinear dynamical phenomena besides multistability such as bifurcations, chaos, and phase synchronization. The degree of multistability can be controlled by an external voltage. In the case of two coexisting states, the system is effectively binary, opening a door to exploitation for developing spintronic memory devices. Because of the dissipationless and spin-momentum locking nature of the surface currents of the topological insulator, little power is needed for generating a significant current, making the system appealing for potential applications in next generation of low power memory devices.
Hybrid Donor-Dot Devices made using Top-down Ion Implantation for Quantum Computing
Bielejec, Edward; Bishop, Nathan; Carroll, Malcolm
2012-02-01
We present progress towards fabricating hybrid donor -- quantum dots (QD) for quantum computing. These devices will exploit the long coherence time of the donor system and the surface state manipulation associated with a QD. Fabrication requires detection of single ions implanted with 10's of nanometer precision. We show in this talk, 100% detection efficiency for single ions using a single ion Geiger mode avalanche (SIGMA) detector integrated into a Si MOS QD process flow. The NanoImplanter (nI) a focused ion beam system is used for precision top-down placement of the implanted ion. This machine has a 10 nm resolution combined with a mass velocity filter, allowing for the use of multi-species liquid metal ion sources (LMIS) to implant P and Sb ions, and a fast blanking and chopping system for single ion implants. The combination of the nI and integration of the SIGMA with the MOS QD process flow establishes a path to fabricate hybrid single donor-dot devices. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.
Color tunable hybrid light-emitting diodes based on perovskite quantum dot/conjugated polymer
Germino, José C.; Yassitepe, Emre; Freitas, Jilian N.; Santiago, Glauco M.; Bonato, Luiz Gustavo; de Morais, Andréia; Atvars, Teresa D. Z.; Nogueira, Ana F.
2017-08-01
Inorganic organic metal halide perovskite materials have been investigated for several technological applications, such as photovoltaic cells, lasers, photodetectors and light emitting diodes (LEDs), either in the bulk form or as colloidal nanoparticles. Recently, all inorganic Cesium Lead Halide (CsPbX3, X=Cl,Br, I) perovskite quantum dots (PQDs) were reported with high photoluminescence quantum yield with narrow emission lines in the visible wavelengths. Here, green-emitting perovskite quantum dots (PQDs) prepared by a synthetic method based on a mixture of oleylamine and oleic acid as surfactants were applied in the electroluminescent layer of hybrid LEDs in combination with two different conjugated polymers: polyvinylcarbazole (PVK) or poly(9,9-di-n-octylfluorenyl-2,7-diyl) (PFO). The performance of the diodes and the emission color tuning upon dispersion of different concentrations of the PQDs in the polymer matrix is discussed. The presented approach aims at the combination of the optical properties of the PQDs and their interaction with wide bandgap conjugated polymers, associated with the solution processing ability of these materials.
A hybrid quantum-inspired genetic algorithm for multiobjective flow shop scheduling.
Li, Bin-Bin; Wang, Ling
2007-06-01
This paper proposes a hybrid quantum-inspired genetic algorithm (HQGA) for the multiobjective flow shop scheduling problem (FSSP), which is a typical NP-hard combinatorial optimization problem with strong engineering backgrounds. On the one hand, a quantum-inspired GA (QGA) based on Q-bit representation is applied for exploration in the discrete 0-1 hyperspace by using the updating operator of quantum gate and genetic operators of Q-bit. Moreover, random-key representation is used to convert the Q-bit representation to job permutation for evaluating the objective values of the schedule solution. On the other hand, permutation-based GA (PGA) is applied for both performing exploration in permutation-based scheduling space and stressing exploitation for good schedule solutions. To evaluate solutions in multiobjective sense, a randomly weighted linear-sum function is used in QGA, and a nondominated sorting technique including classification of Pareto fronts and fitness assignment is applied in PGA with regard to both proximity and diversity of solutions. To maintain the diversity of the population, two trimming techniques for population are proposed. The proposed HQGA is tested based on some multiobjective FSSPs. Simulation results and comparisons based on several performance metrics demonstrate the effectiveness of the proposed HQGA.
DEFF Research Database (Denmark)
Liu, Shuiping; Gu, Tianxun; Fu, Jiajia
2014-01-01
In this work, novel hybrid nanosphere vehicles were synthesized for nitric oxide (NO) donating and real-time detection. The hybrid nanosphere vehicles consist of cadmium selenide quantum dots (CdSe QDs) as NO fluorescent probes, and the modified hyperbranched polyether (mHP)-based diazeniumdiolates...... as NO donors, respectively. The nanospheres have spherical outline with dimension of ~ 127 nm. The data of systematic characterization demonstrated that the mHP-based hybrid nanosphere vehicles (QDs-mHP-NO) can release and real-time detect NO with the low limit of 25 nM, based on fluorescence quenching...
Energy Technology Data Exchange (ETDEWEB)
Wang, Liancheng, E-mail: wanglc@semi.ac.cn, E-mail: lzq@semi.ac.cn, E-mail: zh.zhang@hebut.edu.cn [Engineering Product Development Pillar (EPD), Singapore University of Technology & Design (SUTD), 8 Somapah Road, Singapore 487372 (Singapore); Semiconductor Lighting Technology Research and Development Center, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083 (China); Mind Star (Beijing) Technology Co., Ltd., Zhongguancun South Street, Haidian District, No. 45 Hing Fat Building 1001, Beijing 100872 (China); Liu, Zhiqiang, E-mail: wanglc@semi.ac.cn, E-mail: lzq@semi.ac.cn, E-mail: zh.zhang@hebut.edu.cn; Tian, Ying Dong; Yi, Xiaoyan; Wang, Junxi; Li, Jinmin; Wang, Guohong [Semiconductor Lighting Technology Research and Development Center, Institute of Semiconductors, Chinese Academy of Sciences, Beijing 100083 (China); Zhang, Zi-Hui, E-mail: wanglc@semi.ac.cn, E-mail: lzq@semi.ac.cn, E-mail: zh.zhang@hebut.edu.cn [Key Laboratory of Electronic Materials and Devices of Tianjin, School of Electronics and Information Engineering, Hebei University of Technology, Tianjin 300401 (China)
2016-04-14
The effects of graphene on the optical properties of active system, e.g., the InGaN/GaN multiple quantum wells, are thoroughly investigated and clarified. Here, we have investigated the mechanisms accounting for the photoluminescence reduction for the graphene covered GaN/InGaN multiple quantum wells hybrid structure. Compared to the bare multiple quantum wells, the photoluminescence intensity of graphene covered multiple quantum wells showed a 39% decrease after excluding the graphene absorption losses. The responsible mechanisms have been identified with the following factors: (1) the graphene two dimensional hole gas intensifies the polarization field in multiple quantum wells, thus steepening the quantum well band profile and causing hole-electron pairs to further separate; (2) a lower affinity of graphene compared to air leading to a weaker capability to confine the excited hot electrons in multiple quantum wells; and (3) exciton transfer through non-radiative energy transfer process. These factors are theoretically analysed based on advanced physical models of semiconductor devices calculations and experimentally verified by varying structural parameters, such as the indium fraction in multiple quantum wells and the thickness of the last GaN quantum barrier spacer layer.
High-response hybrid quantum dots- 2D conductor phototransistors: recent progress and perspectives
Directory of Open Access Journals (Sweden)
Sablon Kimberly A.
2017-03-01
Full Text Available Having been inspired by the tremendous progress in material nanoscience and device nanoengineering, hybrid phototransistors combine solution processed colloidal semiconductor quantum dots (QDs with graphene or two-dimensional (2D semiconductor materials. Novel detectors demonstrate ultrahigh photoconductive gain, high and selective photoresponse, low noise, and very high responsivity in visible- and near-infrared ranges. The outstanding performance of phototransistors is primarily due to the strong, selective, and size tunable absorption of QDs and fast charge transfer in 2D high mobility conductors. However, the relatively small mobility of QD nanomaterials was a technological barrier, which limited the operating rate of devices. Very recent innovations in detector design and significant progress in QD ligand engineering provide effective tools for further qualitative improvements. This article reviews the recent progress in material science, nanophysics, and device engineering related to hybrid phototransistors. Detectors based on various QD nanomaterials and several 2D conductors are compared, and advantages and disadvantages of various nanomaterials for applications in hybrid phototransistors are identified. We also benchmark the experimental characteristics with model results that establish interrelations and tradeoffs between detector characteristics, such as responsivity, dark and noise currents, the photocarrier lifetime, response, and noise bandwidths. We have shown that the most recent phototransistors demonstrate performance limited by the fundamental generation recombination noise in high gain devices. Interrelation between the dynamic range of the detector and the detector sensitivity is discussed. The review is concluded with a brief discussion of the remaining challenges and possible significant improvements in the performance of hybrid phototransistors.
DEFF Research Database (Denmark)
Liu, Shuiping; Jin, Lanming; Chronakis, Ioannis S.
2014-01-01
In this work, hybrid nanosphere vehicles consisting of cadmium selenide quantum dots (CdSe QDs) were synthesized for nitric oxide (NO) donating and real-time detecting. The nanospheres with QDs being encapsulation have spherical outline with dimension of ~127 nm. The fluorescence properties...
Wu, Xin; Koslowski, Axel; Thiel, Walter
2012-07-10
In this work, we demonstrate that semiempirical quantum chemical calculations can be accelerated significantly by leveraging the graphics processing unit (GPU) as a coprocessor on a hybrid multicore CPU-GPU computing platform. Semiempirical calculations using the MNDO, AM1, PM3, OM1, OM2, and OM3 model Hamiltonians were systematically profiled for three types of test systems (fullerenes, water clusters, and solvated crambin) to identify the most time-consuming sections of the code. The corresponding routines were ported to the GPU and optimized employing both existing library functions and a GPU kernel that carries out a sequence of noniterative Jacobi transformations during pseudodiagonalization. The overall computation times for single-point energy calculations and geometry optimizations of large molecules were reduced by one order of magnitude for all methods, as compared to runs on a single CPU core.
Vacancy formation energy near an edge dislocation: A hybrid quantum-classical study
International Nuclear Information System (INIS)
Tavazza, F.; Wagner, R.; Chaka, A.M.; Levine, L.E.
2005-01-01
In this work, the formation energy of a single vacancy in aluminum at different distances from an edge dislocation core is studied using a new, hybrid ab initio-classical potential methodology. Such an approach allows us to conduct large-scale atomistic simulations with a simple classical potential (embedded atom method (EAM), for instance) while simultaneously using the more accurate ab initio approach (first principles quantum mechanics) for critical embedded regions. The coupling is made through shared shells of atoms where the two atomistic modeling approaches are relaxed in an iterative, self-consistent manner. The small, critical region is relaxed using all electron density functional theory (DFT) and the much larger cell in which this is embedded is relaxed using a minimization algorithm with EAM potentials
Photoelectronic characterization of IgG antibody molecule-quantum dot hybrid as biosensing probe
Energy Technology Data Exchange (ETDEWEB)
Yu, Hye-Weon; Kim, Sung-Jo; Kim, In S [School of Environmental Science and Engineering, Gwangju Institute of Science and Technology (GIST), 261 Cheomdan-gwagiro, Buk-gu, Gwangju 500-712 (Korea, Republic of); Lee, Jinwook; Kim, Sungyoun, E-mail: iskim@gist.ac.kr [Center for Seawater Desalination Plant, Gwangju Institute of Science and Technology (GIST), 261 Cheomdan-gwagiro, Buk-gu, Gwangju 500-712 (Korea, Republic of)
2010-10-22
Quantum dot (QD)-based biomolecule hybrids have recently attracted much attention in specifically identifying and labeling target proteins. In this study, QD encapsulated with immunoglobulin antibodies, as a labeling building block in biosensors, was investigated to clarify the most efficient configuration and photoluminescence behavior. Both the biological recognition capacity and photoluminescence emitting signal of the antibody-coupled nanocrystal were validated through a photoelectrical characterization procedure. Derivation of the optimum number of antibody molecules to be packed onto the QD surface yielded the highest binding capacity for the target antigen. During formation of the bioactive layer, the intrinsic photoluminescence response of the QDs significantly decreased due to photoinduced hole transfer according to their rearranged electronic structure. The thorough study of this assembly provides a validation approach for the careful titration of biosensor probes for optimal reaction kinetics. Furthermore, it contributes to the development of an effective tool for the application and interpretation of QD-based labeling techniques.
Photoelectronic characterization of IgG antibody molecule-quantum dot hybrid as biosensing probe
International Nuclear Information System (INIS)
Yu, Hye-Weon; Kim, Sung-Jo; Kim, In S; Lee, Jinwook; Kim, Sungyoun
2010-01-01
Quantum dot (QD)-based biomolecule hybrids have recently attracted much attention in specifically identifying and labeling target proteins. In this study, QD encapsulated with immunoglobulin antibodies, as a labeling building block in biosensors, was investigated to clarify the most efficient configuration and photoluminescence behavior. Both the biological recognition capacity and photoluminescence emitting signal of the antibody-coupled nanocrystal were validated through a photoelectrical characterization procedure. Derivation of the optimum number of antibody molecules to be packed onto the QD surface yielded the highest binding capacity for the target antigen. During formation of the bioactive layer, the intrinsic photoluminescence response of the QDs significantly decreased due to photoinduced hole transfer according to their rearranged electronic structure. The thorough study of this assembly provides a validation approach for the careful titration of biosensor probes for optimal reaction kinetics. Furthermore, it contributes to the development of an effective tool for the application and interpretation of QD-based labeling techniques.
Study of plasmonics in hybrids made from a quantum emitter and double metallic nanoshell dimer
Guo, Jiaohan; Black, Kevin; Hu, Jiawen; Singh, Mahi
2018-05-01
We developed a theory for the fluorescence (FL) for quantum emitter and double metallic nanoshell dimer hybrids using the density matrix method. The dimer is made from two identical double metallic nanoshells, which are made of a dielectric core, a gold metallic shell and a dielectric spacer layer. The quantum emitters are deposited on the surface of the spacer layers of the dimers due to the electrostatic absorptions. We consider that dimer hybrids are surrounded by biological cells. This can be achieved by injecting them into human or animal cells. The surface plasmon polaritons (SPP) are calculated for the dimer using Maxwell’s equations in the static wave approximation. The calculated SPP energy agrees with experimental data from Zhai et al (2017 Plasmonics 12 263) for the dimer made from a silica core, a gold metallic nanoshell and a silica spacer layer. We have also obtained an analytical expression of the FL using the density matrix method. We compare our theory with FL experimental data from Zhai et al (2017 Plasmonics 12 263) where the FL spectrum was measured by varying the thickness of the spacer layer from 9 nm to 40 nm. A good agreement between theory and experiment is found. We have shown that the enhancement of the FL increases as the thickness of the spacer layer decreases. We have also found that the enhancement of the FL increases as the distance between the double metallic nanoshells in the dimer decreases. These are interesting findings which are consistent with the experiments of Zhai et al (2017 Plasmonics 12 263) and can be used to control the FL enhancement in the FL-based biomedical imaging and cancer treatment. These interesting findings may also be useful in the fabrication of nanosensors and nanoswitches for applications in medicine.
Biocompatible multi-walled carbon nanotube–CdTe quantum dot–polymer hybrids for medical applications
Energy Technology Data Exchange (ETDEWEB)
Baslak, Canan, E-mail: cananbaslak@gmail.com [Advanced Technology Research and Application Center, Selcuk University, 42075 Konya (Turkey); Department of Chemistry, Faculty of Science, Selcuk University, 42075 Konya (Turkey); Demirel Kars, Meltem, E-mail: dmeltem@yahoo.com [Advanced Technology Research and Application Center, Selcuk University, 42075 Konya (Turkey); Sarayonu Vocational High School, Selcuk University, 42430 Konya (Turkey); Karaman, Mustafa; Kus, Mahmut [Advanced Technology Research and Application Center, Selcuk University, 42075 Konya (Turkey); Department of Chemical Engineering, Faculty of Engineering, Selcuk University, 42075 Konya (Turkey); Cengeloglu, Yunus; Ersoz, Mustafa [Advanced Technology Research and Application Center, Selcuk University, 42075 Konya (Turkey); Department of Chemistry, Faculty of Science, Selcuk University, 42075 Konya (Turkey)
2015-04-15
Herein we report the synthesis of polymer coated quantum dots (QDs)–carbon nanotube composite material with high biocompatibility and low cellular toxicity. The synthesized multi-walled carbon nanotube (MWCNT)–QD-(-poly(glycidyl methacrylate)) (pGMA) hybrids were characterized using X-ray photoelectron spectroscopy, laser scanning confocal microscopy, transmission electron microscopy and scanning electron microscopy. The results showed that quantum dots were well-distributed on nanotube surfaces in high density. The toxicological assessments of QDs and MWCNT–QD–polymer hybrids in human mammary carcinoma cells and their fluorescence imaging in living cell system were carried out. MWCNT–QD–polymer hybrids possess intense red fluorescence signal under confocal microscopy and good fluorescence stability over 6-h exposure in living cell system. The toxicity comparison of QDs and MWCNT–QD–polymer hybrids has shown that the existence of PGMA thin coating on MWCNT–QD hybrid surface decreased the cellular toxicity and increased biocompatibility. - Highlights: • We report that polymer coating of QDs on CNTs increased their biocompatibility by decreasing cellular toxicity. • QD–CNT polymer hybrid material may be proposed as a good diagnostic agent to visualize cancer cells which may be improved as a therapeutic carrier in future. • Coating QDs with polymer seems to be a right choice to be used in medicinal applications both for diagnosis and for therapy.
Energy Technology Data Exchange (ETDEWEB)
Yuan Ying; Riehle, Frank-Stefan [Freiburg Materials Research Centre (FMF), University of Freiburg, Stefan-Meier-Str. 21, D-79104 Freiburg (Germany); Department of Microsystems Engineering (IMTEK), Georg Koehler Allee 103, University of Freiburg, D-79110 Freiburg (Germany); Nitschke, Roland [Life Imaging Center, Centre of Systems Biology, University of Freiburg Habsburgerstr. 49, D-79104 Freiburg (Germany); Centre for Biological Signalling Studies (BIOSS), University of Freiburg (Germany); Krueger, Michael, E-mail: michael.krueger@fmf.uni-freiburg.de [Freiburg Materials Research Centre (FMF), University of Freiburg, Stefan-Meier-Str. 21, D-79104 Freiburg (Germany); Department of Microsystems Engineering (IMTEK), Georg Koehler Allee 103, University of Freiburg, D-79110 Freiburg (Germany)
2012-02-15
Highlights: Black-Right-Pointing-Pointer A novel in situ synthesis approach for highly luminescent CdSe core QDs-nylon hybrid materials. Black-Right-Pointing-Pointer Potential applications for light and energy conversion are demonstrated. Black-Right-Pointing-Pointer Three dimensional structures out of this hybrid material are available. - Abstract: Highly photoluminescent hexadecylamine (HDA) capped core CdSe quantum dots (QDs) with fluorescent quantum yields (QYs) up to 60% were synthesized using a hot injection method and directly incorporated into nylon polymer. For the incorporation of crude CdSe QDs into nylon a simple reproducible and upscalable one pot approach was developed without the need of further purification steps. The photoluminescence (PL) properties of the core QDs and the resulting QD-polymer hybrid composites were investigated and compared. Red emitting hybrid materials exhibit a QY of 60% with a high potential for applications in direct light and energy conversion. The hybrid materials could be successfully utilized as LED conversion layers. By avoiding exposure to oxygen the hybrid films can be kept for a month without detecting a significant decrease in luminescence. Various three dimensional structures are easily available opening doors for further applications such as novel materials for fluorescence standard development in laser scanning microscopy (LSM).
Biocompatible multi-walled carbon nanotube–CdTe quantum dot–polymer hybrids for medical applications
International Nuclear Information System (INIS)
Baslak, Canan; Demirel Kars, Meltem; Karaman, Mustafa; Kus, Mahmut; Cengeloglu, Yunus; Ersoz, Mustafa
2015-01-01
Herein we report the synthesis of polymer coated quantum dots (QDs)–carbon nanotube composite material with high biocompatibility and low cellular toxicity. The synthesized multi-walled carbon nanotube (MWCNT)–QD-(-poly(glycidyl methacrylate)) (pGMA) hybrids were characterized using X-ray photoelectron spectroscopy, laser scanning confocal microscopy, transmission electron microscopy and scanning electron microscopy. The results showed that quantum dots were well-distributed on nanotube surfaces in high density. The toxicological assessments of QDs and MWCNT–QD–polymer hybrids in human mammary carcinoma cells and their fluorescence imaging in living cell system were carried out. MWCNT–QD–polymer hybrids possess intense red fluorescence signal under confocal microscopy and good fluorescence stability over 6-h exposure in living cell system. The toxicity comparison of QDs and MWCNT–QD–polymer hybrids has shown that the existence of PGMA thin coating on MWCNT–QD hybrid surface decreased the cellular toxicity and increased biocompatibility. - Highlights: • We report that polymer coating of QDs on CNTs increased their biocompatibility by decreasing cellular toxicity. • QD–CNT polymer hybrid material may be proposed as a good diagnostic agent to visualize cancer cells which may be improved as a therapeutic carrier in future. • Coating QDs with polymer seems to be a right choice to be used in medicinal applications both for diagnosis and for therapy
Separability in Distant Jauch-Type Hybrid Macrostates of a Quantum and a Classical System
Herbut, Fedor
1986-12-01
It is assumed that for a quantum system ( Q) plus a classical one ( C) that are in a distant state the actually measurable Hermitian operators are of the form A⊗∑ k⌆K b k Q k ( A is any Hermitian operator for Q, and the decomposition ∑ k Q k =1 of the identity is, after von Neumann, characteristic for C). This leads to Jauch-type macrostates (classes of microstates or statistical operators) for Q+C. On the other hand, it is shown that in the Q+Q case the essence of quantum correlations are the conditional states (or statistical operators) of subsystem I and the reduced state ρ II. Along these lines, the correlation entities (as a complete set of invariants) for the macrostates of the Q+C system are derived, and it is shown that one can make an isomorphic transition from the σ-convex set of the latter to that of the hybrid macrostates ( ρ k , p k ) Here ρ k is the conditional state of Q under the condition that Q k occurs on C, and p k is a classical discrete probability distribution on K, taking the place of ρ II as the macrostate of C. This study indirectly throws new light on the nonseparability in the Q+Q case by contrasting it with a well-understood separability in the C+C and Q+C cases.
Directory of Open Access Journals (Sweden)
Weidong Lei
2017-01-01
Full Text Available We aim at solving the cyclic scheduling problem with a single robot and flexible processing times in a robotic flow shop, which is a well-known optimization problem in advanced manufacturing systems. The objective of the problem is to find an optimal robot move sequence such that the throughput rate is maximized. We propose a hybrid algorithm based on the Quantum-Inspired Evolutionary Algorithm (QEA and genetic operators for solving the problem. The algorithm integrates three different decoding strategies to convert quantum individuals into robot move sequences. The Q-gate is applied to update the states of Q-bits in each individual. Besides, crossover and mutation operators with adaptive probabilities are used to increase the population diversity. A repairing procedure is proposed to deal with infeasible individuals. Comparison results on both benchmark and randomly generated instances demonstrate that the proposed algorithm is more effective in solving the studied problem in terms of solution quality and computational time.
Mohammadzadeh, Atefeh; Miri, MirFaez
2018-01-01
We study the response of a semiconductor quantum dot-metal nanoparticle system to an external field E 0 cos ( ω t ) . The borders between Fano, double peaks, weak transition, strong transition, and bistability regions of the phase diagram move considerably as one regards the multipole effects. The exciton-induced transparency is an artifact of the dipole approximation. The absorption of the nanoparticle, the population inversion of the quantum dot, the upper and lower limits of intensity where bistability occurs, the characteristic time to reach the steady state, and other features of the hybrid system change due to the multipole effects. The phase diagrams corresponding to the fields parallel and perpendicular to the axis of system are quite distinguishable. Thus, both the intensity and the polarization of the incident field can be used to control the system. In particular, the incident polarization can be used to switch on and switch off the bistable behavior. For applications such as miniaturized bistable devices and nanosensors sensitive to variations of the dielectric constant of the surrounding medium, multipole effects must be considered.
Effect of graphene on photoluminescence properties of graphene/GeSi quantum dot hybrid structures
International Nuclear Information System (INIS)
Chen, Y. L.; Ma, Y. J.; Wang, W. Q.; Ding, K.; Wu, Q.; Fan, Y. L.; Yang, X. J.; Zhong, Z. Y.; Jiang, Z. M.; Chen, D. D.; Xu, F.
2014-01-01
Graphene has been discovered to have two effects on the photoluminescence (PL) properties of graphene/GeSi quantum dot (QD) hybrid structures, which were formed by covering monolayer graphene sheet on the multilayer ordered GeSi QDs sample surfaces. At the excitation of 488 nm laser line, the hybrid structure had a reduced PL intensity, while at the excitation of 325 nm, it had an enhanced PL intensity. The attenuation in PL intensity can be attributed to the transferring of electrons from the conducting band of GeSi QDs to the graphene sheet. The electron transfer mechanism was confirmed by the time resolved PL measurements. For the PL enhancement, a mechanism called surface-plasmon-polariton (SPP) enhanced absorption mechanism is proposed, in which the excitation of SPP in the graphene is suggested. Due to the resonant excitation of SPP by incident light, the absorption of incident light is much enhanced at the surface region, thus leading to more exciton generation and a PL enhancement in the region. The results may be helpful to provide us a way to improve optical properties of low dimensional surface structures.
International Nuclear Information System (INIS)
Mihalache, Iuliana; Radoi, Antonio; Mihaila, Mihai; Munteanu, Cornel; Marin, Alexandru; Danila, Mihai; Kusko, Mihaela; Kusko, Cristian
2015-01-01
Highlights: • We report a one pot synthesis metod of GQD with controlled size and optoelectronic properties. • An improvement of common N3-DSSC characteristics is achieved when GQDs are used as co-sensitiser. • The role of GQD as cosensitisers in hybrid DSSC was investigated and the interplay between charge and energy transfer phenomena mediated by GQDs was demonstrated. • The GQDs presence determines an inhibition of the recombination processes at the TiO 2 /electrolyte interface. - Abstract: We explored the role of graphene quantum dots (GQDs) as co-sensitizers in hybrid dye sensitized solar cell (DSSC) architectures, focusing on various concurring mechanisms, such as: charge transfer, energy transfer and recombination rate, towards light harvesting improvement. GQDs were prepared by the hydrothermal method that allows the tuning of electronic levels and optical properties by employing appropriate precursors and synthesis conditions. The aim was to realize a type II alignment for TiO 2 /GQD/dye hybrid configuration, using standard N3 Ru-dye in order to improve charge transfer. When GQDs were used as co-sensitizers together with N3 Ru-dye, an improvement in power conversion efficiency was achieved, as shown by electrical measurements. The experimental analysis indicates that this improvement arises from the interplay of various mechanisms mediated by GQDs: (i) enhancement of charge separation and collection due to the cascaded alignment of the energy levels; (ii) energy transfer from GQDs to N3 Ru-dye due to the overlap between GQD photoluminescence and N3 Ru-dye absorption spectra; and (iii) reduction of the electron recombination to the redox couple due to the inhibition of the back electron transfer to the electrolyte by the GQDs
International Nuclear Information System (INIS)
Motazedifard, Ali; Bemani, F; Naderi, M H; Roknizadeh, R; Vitali, D
2016-01-01
We propose and analyse a feasible experimental scheme for a quantum force sensor based on the elimination of backaction noise through coherent quantum noise cancellation (CQNC) in a hybrid atom-cavity optomechanical setup assisted with squeezed vacuum injection. The force detector, which allows for a continuous, broadband detection of weak forces well below the standard quantum limit (SQL), is formed by a single optical cavity simultaneously coupled to a mechanical oscillator and to an ensemble of ultracold atoms. The latter acts as a negative-mass oscillator so that atomic noise exactly cancels the backaction noise from the mechanical oscillator due to destructive quantum interference. Squeezed vacuum injection enforces this cancellation and allows sub-SQL sensitivity to be reached in a very wide frequency band, and at much lower input laser powers. (paper)
Motazedifard, Ali; Bemani, F.; Naderi, M. H.; Roknizadeh, R.; Vitali, D.
2016-07-01
We propose and analyse a feasible experimental scheme for a quantum force sensor based on the elimination of backaction noise through coherent quantum noise cancellation (CQNC) in a hybrid atom-cavity optomechanical setup assisted with squeezed vacuum injection. The force detector, which allows for a continuous, broadband detection of weak forces well below the standard quantum limit (SQL), is formed by a single optical cavity simultaneously coupled to a mechanical oscillator and to an ensemble of ultracold atoms. The latter acts as a negative-mass oscillator so that atomic noise exactly cancels the backaction noise from the mechanical oscillator due to destructive quantum interference. Squeezed vacuum injection enforces this cancellation and allows sub-SQL sensitivity to be reached in a very wide frequency band, and at much lower input laser powers.
Analysis of hybrid mode-locking of two-section quantum dot lasers operating at 1.5 microm.
Heck, Martijn J R; Salumbides, Edcel J; Renault, Amandine; Bente, Erwin A J M; Oei, Yok-Siang; Smit, Meint K; van Veldhoven, René; Nötzel, Richard; Eikema, Kjeld S E; Ubachs, Wim
2009-09-28
For the first time a detailed study of hybrid mode-locking in two-section InAs/InP quantum dot Fabry-Pérot-type lasers is presented. The output pulses have a typical upchirp of approximately 8 ps/nm, leading to very elongated pulses. The mechanism leading to this typical pulse shape and the phase noise is investigated by detailed radio-frequency and optical spectral studies as well as time-domain studies. The pulse shaping mechanism in these lasers is found to be fundamentally different than the mechanism observed in conventional mode-locked laser diodes, based on quantum well gain or bulk material.
Pradeesh, K.; Baumberg, J. J.; Prakash, G. Vijaya
2009-07-01
Thin films of self-organized quantum wells of inorganic-organic hybrid perovskites of (C6H9C2H4NH3)2PbI4 are formed from a simple intercalation strategy to yield well-ordered uniform films over centimeter-size scales. These films compare favorably with traditional solution-chemistry-synthesized thin films. The hybrid films show strong room-temperature exciton-related absorption and photoluminescence, which shift with fabrication protocol. We demonstrate the potential of this method for electronic and photonic device applications.
International Nuclear Information System (INIS)
Sinha, Subhojyoti; Chatterjee, Sanat Kumar; Meikap, Ajit Kumar; Ghosh, Jiten
2014-01-01
Here we report a comparative study on the dielectric relaxation and ac conductivity behaviour of pure polyvinyl alcohol (PVA) and PVA–mercury selenide (HgSe) quantum dot hybrid films in the temperature range 298 K ⩽ T ⩽ 420 K and in the frequency range 100 Hz ⩽ f ⩽ 1 MHz. The prepared nanocomposite exhibits a larger dielectric constant as compared to the pure PVA. The real and imaginary parts of the dielectric constants were found to fit appreciably with the modified Cole–Cole equation, from which temperature-dependent values of the relaxation times, free charge carrier conductivity and space charge carrier conductivity were calculated. The relaxation time decreases with the quantum dot's inclusion in the PVA matrix and with an increase in temperature, whereas free charge carrier conductivity and space charge carrier conductivity increases with an increase in temperature. An increase in ac conductivity for the nanocomposites has also been observed, while the charge transport mechanism was found to follow the correlated barrier hopping model in both cases. An easy-path model with a suitable electrical equivalent circuit has been employed to analyse the temperature-dependent impedance spectra. The imaginary part of the complex electric modulus spectra exhibit an asymmetric nature and a non-Debye type of behaviour, which has been elucidated considering a generalized susceptibility function. The electric modulus spectra of the nanocomposite demonstrate a smaller amplitude and broader width, as compared to the pure PVA sample. (paper)
Separability in distant Jauch-type hybrid macrostates of a quantum and classical system
International Nuclear Information System (INIS)
Herbut, F.
1986-01-01
It is assumed that for a quantum system (Q) plus a classical one (C) that are in a distant state the actually measurable Hermitian operators are of the form A circle cross Sigma/sub k epsilon K/ b/sub k/Q/sub k/ (A is any Hermitian operator for Q, and the decomposition Sigma/sub k/Q/sub k/ = 1 of the identity is, after von Neumann, characteristic for C). This leads to Jauch-type macrostates (classes of microstates or statistical operators) for Q + C. On the other hand, it is shown that in the Q + Q case the essence of quantum correlations are the conditional states (or statistical operators) of subsystem I and the reduced state rho/sub II/. Along these lines, the correlation entities (as a complete set of invariants) for the macrostates of the Q + C system are derived, and it is shown that one can make an isomorphic transition from the σ-convex set of the latter to that of the hybrid macrostates (rho/sub k/, p/sub k/). Here rho/sub k/ is the conditional state of Q under the condition that Q/sub k/ occurs on C, and p/sub k/ is a classical discrete probability distribution on K, taking the place of rho/sub II/ as the macrostate of C. This study indirectly throws new light on the nonseparability in the Q + Q case by contrasting it with a well-understood separability in the C + C and Q + C cases
Shahmuradyan, Anna; Krull, Ulrich J
2016-03-15
Quantum dots (QDs) have been widely used in chemical and biosensing due to their unique photoelectrical properties and are well suited as donors in fluorescence resonance energy transfer (FRET). Selective hybridization interactions of oligonucleotides on QDs have been determined by FRET. Typically, the QD-FRET constructs have made use of labeled targets or have implemented labeled sandwich format assays to introduce dyes in proximity to the QDs for the FRET process. The intention of this new work is to explore a method to incorporate the acceptor dye into the probe molecule. Thiazole orange (TO) derivatives are fluorescent intercalating dyes that have been used for detection of double-stranded nucleic acids. One such dye system has been reported in which single-stranded oligonucleotide probes were doubly labeled with adjacent thiazole orange derivatives. In the absence of the fully complementary (FC) oligonucleotide target, the dyes form an H-aggregate, which results in quenching of fluorescence emission due to excitonic interactions between the dyes. The hybridization of the FC target to the probe provides for dissociation of the aggregate as the dyes intercalate into the double stranded duplex, resulting in increased fluorescence. This work reports investigation of the dependence of the ratiometric signal on the type of linkage used to conjugate the dyes to the probe, the location of the dye along the length of the probe, and the distance between adjacent dye molecules. The limit of detection for 34mer and 90mer targets was found to be identical and was 10 nM (2 pmol), similar to analogous QD-FRET using labeled oligonucleotide target. The detection system could discriminate a one base pair mismatch (1BPM) target and was functional without substantial compromise of the signal in 75% serum. The 1BPM was found to reduce background signal, indicating that the structure of the mismatch affected the environment of the intercalating dyes.
Tsai, Meng Lin; Wei, Wan-Rou; Tang, Libin; Chang, Hung Chih; Tai, Shih Hsiang; Yang, Po Kang; Lau, Shu Ping; Chen, Lih Juann; He, Jr-Hau
2015-01-01
By employing graphene quantum dots (GQDs) in PEDOT:PSS, we have achieved an efficiency of 13.22% in Si/PEDOT:PSS hybrid solar cells. The efficiency enhancement is based on concurrent improvement in optical and electrical properties by the photon downconversion process and the improved conductivity of PEDOT:PSS via appropriate incorporation of GQDs. After introducing GQDs into PEDOT:PSS, the short circuit current and the fill factor of rear-contact optimized hybrid cells are increased from 32.11 to 36.26 mA/cm and 62.85% to 63.87%, respectively. The organic-inorganic hybrid solar cell obtained herein holds the promise for developing photon-managing, low-cost, and highly efficient photovoltaic devices.
Tsai, Meng Lin
2015-12-18
By employing graphene quantum dots (GQDs) in PEDOT:PSS, we have achieved an efficiency of 13.22% in Si/PEDOT:PSS hybrid solar cells. The efficiency enhancement is based on concurrent improvement in optical and electrical properties by the photon downconversion process and the improved conductivity of PEDOT:PSS via appropriate incorporation of GQDs. After introducing GQDs into PEDOT:PSS, the short circuit current and the fill factor of rear-contact optimized hybrid cells are increased from 32.11 to 36.26 mA/cm and 62.85% to 63.87%, respectively. The organic-inorganic hybrid solar cell obtained herein holds the promise for developing photon-managing, low-cost, and highly efficient photovoltaic devices.
An All-Solution-Based Hybrid CMOS-Like Quantum Dot/Carbon Nanotube Inverter.
Shulga, Artem G; Derenskyi, Vladimir; Salazar-Rios, Jorge Mario; Dirin, Dmitry N; Fritsch, Martin; Kovalenko, Maksym V; Scherf, Ullrich; Loi, Maria A
2017-09-01
The development of low-cost, flexible electronic devices is subordinated to the advancement in solution-based and low-temperature-processable semiconducting materials, such as colloidal quantum dots (QDs) and single-walled carbon nanotubes (SWCNTs). Here, excellent compatibility of QDs and SWCNTs as a complementary pair of semiconducting materials for fabrication of high-performance complementary metal-oxide-semiconductor (CMOS)-like inverters is demonstrated. The n-type field effect transistors (FETs) based on I - capped PbS QDs (V th = 0.2 V, on/off = 10 5 , S S-th = 114 mV dec -1 , µ e = 0.22 cm 2 V -1 s -1 ) and the p-type FETs with tailored parameters based on low-density random network of SWCNTs (V th = -0.2 V, on/off > 10 5 , S S-th = 63 mV dec -1 , µ h = 0.04 cm 2 V -1 s -1 ) are integrated on the same substrate in order to obtain high-performance hybrid inverters. The inverters operate in the sub-1 V range (0.9 V) and have high gain (76 V/V), large maximum-equal-criteria noise margins (80%), and peak power consumption of 3 nW, in combination with low hysteresis (10 mV). © 2017 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Black Phosphorus Quantum Dots for Hole Extraction of Typical Planar Hybrid Perovskite Solar Cells.
Chen, Wei; Li, Kaiwen; Wang, Yao; Feng, Xiyuan; Liao, Zhenwu; Su, Qicong; Lin, Xinnan; He, Zhubing
2017-02-02
Black phosphorus, famous as two-dimensional (2D) materials, shows such excellent properties for optoelectronic devices such as tunable direct band gap, extremely high hole mobility (300-1000 cm 2 /(V s)), and so forth. In this Letter, facile processed black phosphorus quantum dots (BPQDs) were successfully applied to enhance hole extraction at the anode side of the typical p-i-n planar hybrid perovskite solar cells, which remarkably improved the performance of devices with photon conversion efficiency ramping up from 14.10 to 16.69%. Moreover, more detailed investigations by c-AFM, SKPM, SEM, hole-only devices, and photon physics measurements discover further the hole extraction effect and work mechanism of the BPQDs, such as nucleation assistance for the growth of large grain size perovskite crystals, fast hole extraction, more efficient hole transfer, and suppression of energy-loss recombination at the anode interface. This work definitely paves the way for discovering more and more 2D materials with high electronic properties to be used in photovoltaics and optoelectronics.
Semi-classical description of matter wave interferometers and hybrid quantum systems
Energy Technology Data Exchange (ETDEWEB)
Schneider, Mathias
2015-02-16
This work considers the semi-classical description of two applications involving cold atoms. This is, on one hand, the behavior of a BOSE-EINSTEIN condensate in hybrid systems, i.e. in contact with a microscopic object (carbon nanotubes, fullerenes, etc.). On the other, the evolution of phase space distributions in matter wave interferometers utilizing ray tracing methods was discussed. For describing condensates in hybrid systems, one can map the GROSS-PITAEVSKII equation, a differential equation in the complex-valued macroscopic wave function, onto a system of two differential equations in density and phase. Neglecting quantum dispersion, one obtains a semiclassical description which is easily modified to incorporate interactions between condensate and microscopical object. In our model, these interactions comprise attractive forces (CASIMIR-POLDER forces) and loss of condensed atoms due to inelastic collisions at the surface of the object. Our model exhibited the excitation of sound waves that are triggered by the object's rapid immersion, and spread across the condensate thereafter. Moreover, local particle loss leads to a shrinking of the bulk condensate. We showed that the total number of condensed particles is decreasing potentially in the beginning (large condensate, strong mean field interaction), while it decays exponentially in the long-time limit (small condensate, mean field inetraction negligible). For representing the physics of matter wave interferometers in phase space, we utilized the WIGNER function. In semi-classical approximation, which again consists in ignoring the quantum dispersion, this representation is subject to the same equation of motion as classical phase space distributions, i.e. the LIOUVILLE equation. This implies that time evolution of theWIGNER function follows a phase space flow that consists of classical trajectories (classical transport). This means, for calculating a time-evolved distribution, one has know the initial
Directory of Open Access Journals (Sweden)
Francis S. Maloney
2016-10-01
Full Text Available Zinc oxide nanowire and titanium dioxide nanoparticle (ZnO:TiO2 NW/NP hybrid films were utilized as the photoanode layer in quantum dot-sensitized solar cells (QDSSCs. CdSe quantum dots (QDs with a ZnS passivation layer were deposited on the ZnO:TiO2 NW/NP layer as a photosensitizer by successive ion layer adsorption and reaction (SILAR. Cells were fabricated using a solid-state polymer electrolyte and intensity-modulated photovoltage and photocurrent spectroscopy (IMVS/PS was carried out to study the electron transport properties of the cell. Increasing the SILAR coating number enhanced the total charge collection efficiency of the cell. The electron transport time constant and diffusion length were found to decrease as more QD layers were added.
Elizaga Navascués, Beatriz; Martín de Blas, Daniel; Mena Marugán, Guillermo A.
2018-02-01
Loop quantum cosmology has recently been applied in order to extend the analysis of primordial perturbations to the Planck era and discuss the possible effects of quantum geometry on the cosmic microwave background. Two approaches to loop quantum cosmology with admissible ultraviolet behavior leading to predictions that are compatible with observations are the so-called hybrid and dressed metric approaches. In spite of their similarities and relations, we show in this work that the effective equations that they provide for the evolution of the tensor and scalar perturbations are somewhat different. When backreaction is neglected, the discrepancy appears only in the time-dependent mass term of the corresponding field equations. We explain the origin of this difference, arising from the distinct quantization procedures. Besides, given the privileged role that the big bounce plays in loop quantum cosmology, e.g. as a natural instant of time to set initial conditions for the perturbations, we also analyze the positivity of the time-dependent mass when this bounce occurs. We prove that the mass of the tensor perturbations is positive in the hybrid approach when the kinetic contribution to the energy density of the inflaton dominates over its potential, as well as for a considerably large sector of backgrounds around that situation, while this mass is always nonpositive in the dressed metric approach. Similar results are demonstrated for the scalar perturbations in a sector of background solutions that includes the kinetically dominated ones; namely, the mass then is positive for the hybrid approach, whereas it typically becomes negative in the dressed metric case. More precisely, this last statement is strictly valid when the potential is quadratic for values of the inflaton mass that are phenomenologically favored.
Guo, L. Jay
2015-10-01
adopted by other material systems as well. Based on these understandings, we have also developed colored perovskite PV by integrating an optical cavity with the perovskite semiconductors [4]. The principle and experimental results will be presented. 1. J. Y. Lee, K. T. Lee, S.Y. Seo, L. J. Guo, "Decorative power generating panels creating angle insensitive transmissive colors," Sci. Rep. 4, 4192, 2014. 2. K. T. Lee, J.Y. Lee, S.-Y. Seo, and L. J. Guo, "Colored ultra-thin hybrid photovoltaics with high quantum efficiency," Light: Science and Applications, 3, e215, 2014. 3. K. T. Lee, S.-Y. Seo, J.Y. Lee, and L. J. Guo, "Ultrathin metal-semiconductor-metal resonator for angle invariant visible band transmission filters," Appl. Phys. Lett. 104, 231112, (2014); and "Strong resonance effect in a lossy medium-based optical cavity for angle robust spectrum filters," Adv. Mater, 26, 6324-6328, 2014. 4. K. T. Lee, M. Fukuda, L. J. Guo, "Colored, see-through perovskite solar cells employing an optical cavity," Submitted, 2015
Directory of Open Access Journals (Sweden)
Yong Wang
2014-01-01
Full Text Available In order to increase the driving range and improve the overall performance of all-electric vehicles, a new dual-motor hybrid driving system with two power sources was proposed. This system achieved torque-speed coupling between the two power sources and greatly improved the high performance working range of the motors; at the same time, continuously variable transmission (CVT was achieved to efficiently increase the driving range. The power system parameters were determined using the “global optimization method”; thus, the vehicle’s dynamics and economy were used as the optimization indexes. Based on preliminary matches, quantum genetic algorithm was introduced to optimize the matching in the dual-motor hybrid power system. Backward simulation was performed on the combined simulation platform of Matlab/Simulink and AVL-Cruise to optimize, simulate, and verify the system parameters of the transmission system. Results showed that quantum genetic algorithms exhibited good global optimization capability and convergence in dealing with multiobjective and multiparameter optimization. The dual-motor hybrid-driving system for electric cars satisfied the dynamic performance and economy requirements of design, efficiently increasing the driving range of the car, having high performance, and reducing energy consumption of 15.6% compared with the conventional electric vehicle with single-speed reducers.
A hybrid lattice basis reduction and quantum search attack on LWE
Göpfert, F.; Van Vredendaal, C.; Wunderer, T.
2017-01-01
Recently, an increasing amount of papers proposing post-quantum schemes also provide concrete parameter sets aiming for concrete post-quantum security levels. Security evaluations of such schemes need to include all possible attacks, in particular those by quantum adversaries. In the case of
Hybridization of electron states in a step quantum well in a magnetic field
International Nuclear Information System (INIS)
Barseghyan, M.G.; Kirakosyan, A.A.
2005-01-01
The quantum states and energy levels of an electrion in a rectangular step quantum well in a magnetic field parallel to the plane of two-dimentional electron gas are investigated. It is shown that the joint effect of the magnetic field and confining potential of the quantum well results in redical change of the electron spectrum. The dependence of the electron energy levels on the quantum well parameters, magnetic field induction and projection of the wave-vector along the magnetic field induction are calculated. Numerical calculations are carried out for a AlAs/GaAlAs/GaAs/AlAs step quantum well
International Nuclear Information System (INIS)
Lipparini, Filippo; Scalmani, Giovanni; Frisch, Michael J.; Lagardère, Louis; Stamm, Benjamin; Cancès, Eric; Maday, Yvon; Piquemal, Jean-Philip; Mennucci, Benedetta
2014-01-01
We present the general theory and implementation of the Conductor-like Screening Model according to the recently developed ddCOSMO paradigm. The various quantities needed to apply ddCOSMO at different levels of theory, including quantum mechanical descriptions, are discussed in detail, with a particular focus on how to compute the integrals needed to evaluate the ddCOSMO solvation energy and its derivatives. The overall computational cost of a ddCOSMO computation is then analyzed and decomposed in the various steps: the different relative weights of such contributions are then discussed for both ddCOSMO and the fastest available alternative discretization to the COSMO equations. Finally, the scaling of the cost of the various steps with respect to the size of the solute is analyzed and discussed, showing how ddCOSMO opens significantly new possibilities when cheap or hybrid molecular mechanics/quantum mechanics methods are used to describe the solute
Energy Technology Data Exchange (ETDEWEB)
Lipparini, Filippo, E-mail: flippari@uni-mainz.de [Sorbonne Universités, UPMC Univ. Paris 06, UMR 7598, Laboratoire Jacques-Louis Lions, F-75005 Paris (France); Sorbonne Universités, UPMC Univ. Paris 06, UMR 7616, Laboratoire de Chimie Théorique, F-75005 Paris (France); Sorbonne Universités, UPMC Univ. Paris 06, Institut du Calcul et de la Simulation, F-75005 Paris (France); Scalmani, Giovanni; Frisch, Michael J. [Gaussian, Inc., 340 Quinnipiac St. Bldg. 40, Wallingford, Connecticut 06492 (United States); Lagardère, Louis [Sorbonne Universités, UPMC Univ. Paris 06, Institut du Calcul et de la Simulation, F-75005 Paris (France); Stamm, Benjamin [Sorbonne Universités, UPMC Univ. Paris 06, UMR 7598, Laboratoire Jacques-Louis Lions, F-75005 Paris (France); CNRS, UMR 7598 and 7616, F-75005 Paris (France); Cancès, Eric [Université Paris-Est, CERMICS, Ecole des Ponts and INRIA, 6 and 8 avenue Blaise Pascal, 77455 Marne-la-Vallée Cedex 2 (France); Maday, Yvon [Sorbonne Universités, UPMC Univ. Paris 06, UMR 7598, Laboratoire Jacques-Louis Lions, F-75005 Paris (France); Institut Universitaire de France, Paris, France and Division of Applied Maths, Brown University, Providence, Rhode Island 02912 (United States); Piquemal, Jean-Philip [Sorbonne Universités, UPMC Univ. Paris 06, UMR 7616, Laboratoire de Chimie Théorique, F-75005 Paris (France); CNRS, UMR 7598 and 7616, F-75005 Paris (France); Mennucci, Benedetta [Dipartimento di Chimica e Chimica Industriale, Università di Pisa, Via Risorgimento 35, 56126 Pisa (Italy)
2014-11-14
We present the general theory and implementation of the Conductor-like Screening Model according to the recently developed ddCOSMO paradigm. The various quantities needed to apply ddCOSMO at different levels of theory, including quantum mechanical descriptions, are discussed in detail, with a particular focus on how to compute the integrals needed to evaluate the ddCOSMO solvation energy and its derivatives. The overall computational cost of a ddCOSMO computation is then analyzed and decomposed in the various steps: the different relative weights of such contributions are then discussed for both ddCOSMO and the fastest available alternative discretization to the COSMO equations. Finally, the scaling of the cost of the various steps with respect to the size of the solute is analyzed and discussed, showing how ddCOSMO opens significantly new possibilities when cheap or hybrid molecular mechanics/quantum mechanics methods are used to describe the solute.
Algar, W Russ; Krull, Ulrich J
2009-01-06
Fluorescence resonance energy transfer (FRET) using immobilized quantum dots (QDs) as energy donors was explored as a transduction method for the detection of nucleic acid hybridization at an interface. This research was motivated by the success of the QD-FRET-based transduction of nucleic acid hybridization in solution-phase assays. This new work represents a fundamental step toward the assembly of a biosensor, where immobilization of the selective chemistry on a surface is desired. After immobilizing QD-probe oligonucleotide conjugates on optical fibers, a demonstration of the retention of selectivity was achieved by the introduction of acceptor (Cy3)-labeled single-stranded target oligonucleotides. Hybridization generated the proximity required for FRET, and the resulting fluorescence spectra provided an analytical signal proportional to the amount of target. This research provides an important framework for the future development of nucleic acid biosensors based on QDs and FRET. The most important findings of this work are that (1) a QD-FRET solid-phase hybridization assay is viable and (2) a passivating layer of denatured bovine serum albumin alleviates nonspecific adsorption, ultimately resulting in (3) the potential for a reusable assay format and mismatch discrimination. In this, the first incarnation of a solid-phase QD-FRET hybridization assay, the limit of detection was found to be 5 nM, and the dynamic range was almost 2 orders of magnitude. Selective discrimination of the target was shown using a three-base-pairs mismatch from a fully complementary sequence. Despite a gradual loss of signal, reuse of the optical fibers over multiple cycles of hybridization and dehybridization was possible. Directions for further improvement of the analytical performance by optimizing the design of the QD-probe oligonucleotide interface are identified.
International Nuclear Information System (INIS)
Nizamoglu, Sedat; Mutlugun, Evren; Akyuz, Ozgun; Perkgoz, Nihan Kosku; Demir, Hilmi Volkan; Liebscher, Lydia; Sapra, Sameer; Gaponik, Nikolai; Eychmueller, Alexander
2008-01-01
To generate white light using semiconductor nanocrystal (NC) quantum dots integrated on light emitting diodes (LEDs), multiple hybrid device parameters (emission wavelengths of the NCs and the excitation platform, order of the NCs with different sizes, amount of the different types of NCs, etc) need to be carefully designed and properly implemented. In this study, we introduce and demonstrate white LEDs based on simple device hybridization using only a single type of white emitting CdS quantum dot nanoluminophores on near-ultraviolet LEDs. Here we present their design, synthesis-growth, fabrication and characterization. With these hybrid devices, we achieve high color rendering index (>70), despite using only a single NC type. Furthermore, we conveniently tune their photometric properties including the chromaticity coordinates, correlated color temperature, and color rendering index with the number of hybridized nanoluminophores in a controlled manner
DEFF Research Database (Denmark)
Chen, Miaoxiang Max; Kobashi, Kazufumi
2012-01-01
Hybridizing air-stable organic-molecules with advanced III-V semiconductor quantum-dots (QDs) structures can be utilized to create a new generation of biochemical sensing devices. In order to enhance their optical performances, the active regions in these QDs structures commonly consist of multis......Hybridizing air-stable organic-molecules with advanced III-V semiconductor quantum-dots (QDs) structures can be utilized to create a new generation of biochemical sensing devices. In order to enhance their optical performances, the active regions in these QDs structures commonly consist...
Ni, Limeng; Huynh, Uyen; Cheminal, Alexandre; Thomas, Tudor H; Shivanna, Ravichandran; Hinrichsen, Ture F; Ahmad, Shahab; Sadhanala, Aditya; Rao, Akshay
2017-11-28
Self-assembled hybrid perovskite quantum wells have attracted attention due to their tunable emission properties, ease of fabrication, and device integration. However, the dynamics of excitons in these materials, especially how they couple to phonons, remains an open question. Here, we investigate two widely used materials, namely, butylammonium lead iodide (CH 3 (CH 2 ) 3 NH 3 ) 2 PbI 4 and hexylammonium lead iodide (CH 3 (CH 2 ) 5 NH 3 ) 2 PbI 4 , both of which exhibit broad photoluminescence tails at room temperature. We performed femtosecond vibrational spectroscopy to obtain a real-time picture of the exciton-phonon interaction and directly identified the vibrational modes that couple to excitons. We show that the choice of the organic cation controls which vibrational modes the exciton couples to. In butylammonium lead iodide, excitons dominantly couple to a 100 cm -1 phonon mode, whereas in hexylammonium lead iodide, excitons interact with phonons with frequencies of 88 and 137 cm -1 . Using the determined optical phonon energies, we analyzed photoluminescence broadening mechanisms. At low temperatures (photoluminescence line shape observed in hybrid perovskite quantum wells and provide insights into the mechanism of exciton-phonon coupling in these materials.
International Nuclear Information System (INIS)
Sakko, Arto; Rossi, Tuomas P; Nieminen, Risto M
2014-01-01
The presence of plasmonic material influences the optical properties of nearby molecules in untrivial ways due to the dynamical plasmon-molecule coupling. We combine quantum and classical calculation schemes to study this phenomenon in a hybrid system that consists of a Na 2 molecule located in the gap between two Au/Ag nanoparticles. The molecule is treated quantum-mechanically with time-dependent density-functional theory, and the nanoparticles with quasistatic classical electrodynamics. The nanoparticle dimer has a plasmon resonance in the visible part of the electromagnetic spectrum, and the Na 2 molecule has an electron-hole excitation in the same energy range. Due to the dynamical interaction of the two subsystems the plasmon and the molecular excitations couple, creating a hybridized molecular-plasmon excited state. This state has unique properties that yield e.g. enhanced photoabsorption compared to the freestanding Na 2 molecule. The computational approach used enables decoupling of the mutual plasmon-molecule interaction, and our analysis verifies that it is not legitimate to neglect the backcoupling effect when describing the dynamical interaction between plasmonic material and nearby molecules. Time-resolved analysis shows nearly instantaneous formation of the coupled state, and provides an intuitive picture of the underlying physics. (paper)
Energy Technology Data Exchange (ETDEWEB)
Zhu, Yuhan; Yan, Kai; Liu, Yong; Zhang, Jingdong, E-mail: zhangjd@mail.hust.edu.cn
2015-07-16
Highlights: • Photovoltammetric behavior of PPD on CdS–GS hybrid film was studied. • GS doped in CdS greatly improved the photoelectrochemical response of PPD. • CV of PPD on CdS–GS film became a sigmoidal shape under photoirradiation. • Novel photoelectrochemical strategy for PPD determination was developed. - Abstract: A photoelectroactive film composed of CdS quantum dots and graphene sheets (GS) was coated on F-doped SnO{sub 2} (FTO) conducting glass for studying the electrochemical response of p-phenylenediamine (PPD) under photoirradiation. The result indicated that the cyclic voltammogram of PPD on CdS–GS hybrid film became sigmoidal in shape after exposed under visible light, due to the photoelectrocatalytic reaction. Such a photovoltammetric response was used to rapidly optimize the photoelectrocatalytic activity of hybrid films composed of different ratios of CdS to GS toward PPD. The influences of scan rate and pH on the photovoltammetric behavior of PPD on CdS–GS film revealed that although the controlled step for electrochemical process was not changed under photoirradiation, more electrons than protons might participate the photoelectrocatalytic process. Furthermore, the photoelectroactive CdS–GS hybrid film was explored for PPD determination based on the photocurrent response of film toward PPD. Under optimal conditions, the photocurrent signal on CdS–GS film was linearly proportional to the concentration of PPD ranging from 1.0 × 10{sup −7} to 3.0 × 10{sup −6} mol L{sup −1}, with a detection limit (3S/N) of 4.3 × 10{sup −8} mol L{sup −1}. Our work based on CdS–GS hybrid film not only demonstrated a new facile photovoltammetric way to study the photoinduced electron transfer process of PPD, but also developed a sensitive photoelectrochemical strategy for PPD determination.
Energy Technology Data Exchange (ETDEWEB)
Mehrabian, Masood [Maragheh Univ. (Iran, Islamic Republic of). Faculty of Basic Science; Abdollahian, Parinaz [Maragheh Univ. (Iran, Islamic Republic of). Dept. of Materials Engineering
2016-07-01
PbS Quantum dots and P3HT are promising materials for photovoltaic applications due to their absorption in the NIR and visible region, respectively. Our previous experimental work showed that doping Al to ZnO lattice (Al:ZnO) could efficiently improve the cell performance. In this article, hybrid solar cells containing of two active areas with ITO/Al:ZnO/PbS QDs/P3HT and PCBM/Ag structure were fabricated and the effect of PbS QD size on photovoltaic properties was investigated. Optimised solar cell showed maximum power conversion efficiency of 2.45 % with short-circuit current of 9.36 mA/cm{sup 2} and open-circuit voltage of 0.59 V under 1 sun illumination (AM1.5).
Energy Technology Data Exchange (ETDEWEB)
Hwang, Gyoyeon [Chemical Kinomics Research Center, Future Convergence Research Division, Korea Institute of Science and Technology, Hwarangno 14-gil 5, Seongbuk-gu, Seoul 136-791 (Korea, Republic of); Biological Chemistry, Korea University of Science and Technology, 217, Gajeong-ro, Yuseong-gu, Deajeon (Korea, Republic of); Lee, Hansol [Chemical Kinomics Research Center, Future Convergence Research Division, Korea Institute of Science and Technology, Hwarangno 14-gil 5, Seongbuk-gu, Seoul 136-791 (Korea, Republic of); Lee, Jiyeon, E-mail: jylee@kist.re.kr [Chemical Kinomics Research Center, Future Convergence Research Division, Korea Institute of Science and Technology, Hwarangno 14-gil 5, Seongbuk-gu, Seoul 136-791 (Korea, Republic of); Biological Chemistry, Korea University of Science and Technology, 217, Gajeong-ro, Yuseong-gu, Deajeon (Korea, Republic of)
2015-11-13
The telomere shortening in chromosomes implies the senescence, apoptosis, or oncogenic transformation of cells. Since detecting telomeres in aging and diseases like cancer, is important, the direct detection of telomeres has been a very useful biomarker. We propose a telomere detection method using a newly synthesized quantum dot (QD) based probe with oligonucleotide conjugation and direct fluorescence in situ hybridization (FISH). QD-oligonucleotides were prepared with metal coordination bonding based on platinum-guanine binding reported in our previous work. The QD-oligonucleotide conjugation method has an advantage where any sequence containing guanine at the end can be easily bound to the starting QD-Pt conjugate. A synthesized telomeric oligonucleotide was bound to the QD-Pt conjugate successfully and this probe hybridized specifically on the telomere of fabricated MV-4-11 and MOLT-4 chromosomes. Additionally, the QD-telomeric oligonucleotide probe successfully detected the telomeres on the CGH metaphase slide. Due to the excellent photostability and high quantum yield of QDs, the QD-oligonucleotide probe has high fluorescence intensity when compared to the organic dye-oligonucleotide probe. Our QD-oligonucleotide probe, conjugation method of this QD probe, and hybridization protocol with the chromosomes can be a useful tool for chromosome painting and FISH. - Highlights: • We prepared a probe linked between QD and telomeric oligonucleotide with platinum-guanine bonding. • Telomeres were detected by our new telomere probes successfully in three different human metaphase chromosomes. • QDPt-DNA probe has high fluorescence intensity in comparison with organic dye-DNA probe.
International Nuclear Information System (INIS)
Niu, Fujun; Shen, Shaohua; Wang, Jian; Guo, Liejin
2016-01-01
Graphical abstract: A cobalt complex engineers the interfacial energetics of metal oxide quantum dots (n- or p-type) and electrolytes for highly efficient O_2 generation under visible light irradiation. - Highlights: • A noble-metal-free hybrid photocatalytic system using a single-site cobalt catalyst was developed for O_2 generation. • Considerable activity and excellent stability for O_2 production were achieved by this novel system. • CoSlp engineered the QDs/electrolyte interfacical energetics for efficient hole transfer. - Abstract: Here we reported a novel hybrid photocatalytic water oxidation system, containing metal oxide (n-Fe_2O_3 or p-Co_3O_4) quantum dots (QDs) as light harvester, a salophen cobalt(II) complex (CoSlp) as redox catalyst and persulfate (S_2O_8"2"−) as sacrificial electron acceptor, for oxygen generation from fully aqueous solution. The n-Fe_2O_3 QDs/CoSlp and p-Co_3O_4 QDs/CoSlp systems exhibited good O_2 evolution performances, giving turnover numbers (TONs) of ca. 33 and ca. 35 over CoSlp after visible light irradiation for 72 h, respectively. The excellent photocatalytic performance could be ascribed to the efficient hole transfer from QDs to CoSlp catalyst, leading to reduced photogenerated charge recombination, as well as the CoSlp engineered interfacial band bending of QDs, increasing the driving force or decreasing the energy barrier for hole transfer and then benefiting the following O_2 generation at the QDs/electrolyte interface. The present work successfully demonstrated a novel hybrid system for photocatalytic O_2 evolution from fully aqueous solution; and the essential role of cobalt complexes in engineering the interfacial energetics of semiconductors (n- or p-type) and electrolytes could be informative for designing efficient systems for solar water splitting.
Hybrid InGaAs quantum well-dots nanostructures for light-emitting and photo-voltaic applications.
Mintairov, S A; Kalyuzhnyy, N A; Lantratov, V M; Maximov, M V; Nadtochiy, A M; Rouvimov, Sergei; Zhukov, A E
2015-09-25
Hybrid quantum well-dots (QWD) nanostructures have been formed by deposition of 7-10 monolayers of In0.4Ga0.6As on a vicinal GaAs surface using metal-organic chemical vapor deposition. Transmission electron microscopy, photoluminescence and photocurrent analysis have shown that such structures represent quantum wells comprising three-dimensional (quantum dot-like) regions of two kinds. At least 20 QWD layers can be deposited defect-free providing high gain/absorption in the 0.9-1.1 spectral interval. Use of QWD media in a GaAs solar cell resulted in a photocurrent increment of 3.7 mA cm(-2) for the terrestrial spectrum and by 4.1 mA cm(-2) for the space spectrum. Diode lasers based on QWD emitting around 1.1 μm revealed high saturated gain and low transparency current density of about 15 cm(-1) and 37 A cm(-2) per layer, respectively.
Energy Technology Data Exchange (ETDEWEB)
Liu, Shuiping; Gu, Tianxun; Fu, Jiajia [Key Laboratory of Eco-Textiles, Ministry of Education (Jiangnan University), Wuxi 214122 (China); College of Textile and Clothing, Jiangnan University, Wuxi 214122 (China); Li, Xiaoqiang, E-mail: leecaiwei@163.com [Key Laboratory of Eco-Textiles, Ministry of Education (Jiangnan University), Wuxi 214122 (China); College of Textile and Clothing, Jiangnan University, Wuxi 214122 (China); Technical University of Denmark, DTU Food, Søltofts plads, B227, 2800 Kgs. Lyngby (Denmark); Chronakis, Ioannis S. [Technical University of Denmark, DTU Food, Søltofts plads, B227, 2800 Kgs. Lyngby (Denmark); Ge, Mingqiao [Key Laboratory of Eco-Textiles, Ministry of Education (Jiangnan University), Wuxi 214122 (China); College of Textile and Clothing, Jiangnan University, Wuxi 214122 (China)
2014-12-01
In this work, novel hybrid nanosphere vehicles were synthesized for nitric oxide (NO) donating and real-time detection. The hybrid nanosphere vehicles consist of cadmium selenide quantum dots (CdSe QDs) as NO fluorescent probes, and the modified hyperbranched polyether (mHP)-based diazeniumdiolates as NO donors, respectively. The nanospheres have spherical outline with dimension of ∼ 127 nm. The data of systematic characterization demonstrated that the mHP-based hybrid nanosphere vehicles (QDs-mHP-NO) can release and real-time detect NO with the low limit of 25 nM, based on fluorescence quenching mechanism. The low cell-toxicity of QDs-mHP-NO nanospheres was verified by means of MTT assay on L929 cells viability. The QDs-mHP-NO nanospheres provide perspectives for designing a new class of biocompatible NO donating and imaging systems. - Highlights: • QDs-mHP-NO fluorescent probe was prepared. • The QDs-mHP-NO probe is capable of releasing NO. • The QDs-mHP-NO probe can quantitatively detecting the release of NO in real time. • The low cell-toxicity of QDs-mHP-NO nanospheres was verified.
Chou, Cheng-Chung; Huang, Yi-Han
2012-01-01
This paper reports a nucleic acid sandwich hybridization assay with a quantum dot (QD)-induced fluorescence resonance energy transfer (FRET) reporter system. Two label-free hemagglutinin H5 sequences (60-mer DNA and 630-nt cDNA fragment) of avian influenza viruses were used as the targets in this work. Two oligonucleotides (16 mers and 18 mers) that specifically recognize two separate but neighboring regions of the H5 sequences were served as the capturing and reporter probes, respectively. The capturing probe was conjugated to QD655 (donor) in a molar ratio of 10:1 (probe-to-QD), and the reporter probe was labeled with Alexa Fluor 660 dye (acceptor) during synthesis. The sandwich hybridization assay was done in a 20 μL transparent, adhesive frame-confined microchamber on a disposable, temperature-adjustable indium tin oxide (ITO) glass slide. The FRET signal in response to the sandwich hybridization was monitored by a homemade optical sensor comprising a single 400 nm UV light-emitting diode (LED), optical fibers, and a miniature 16-bit spectrophotometer. The target with a concentration ranging from 0.5 nM to 1 μM was successfully correlated with both QD emission decrease at 653 nm and dye emission increase at 690 nm. To sum up, this work is beneficial for developing a portable QD-based nucleic acid sensor for on-site pathogen detection. PMID:23211753
Kim, Taesoo
2018-05-03
Realization of colloidal quantum dot (CQD)/organic photovoltaic (OPV) tandem solar cells that integrate the strong infrared absorption of CQDs with large photovoltages of OPVs is an attractive option toward high-performing, low-cost thin film solar cells. To date, monolithic hybrid tandem integration of CQD/OPV solar cells has been restricted due to the CQD ink’s catastrophic damage to the organic subcell, thus forcing the low bandgap CQD to be used as front cell. This sub-optimal configuration limits the maximum achievable photocurrent in CQD/OPV hybrid tandem solar cells. In this work, we demonstrate hybrid tandem solar cells employing a low-bandgap CQD back cell on top of an organic front cell thanks to a modified CQD ink formulation and a robust interconnection layer (ICL) which together overcome the long-standing integration challenges for CQD and organic subcells. The resulting tandem architecture surpasses previously reported current densities by ~20-25% and yields a state-of-the-art power conversion efficiency (PCE) of 9.4%.
Tsai, Meng-Lin
2017-04-21
Despite great improvements in traditional inorganic photodetectors and photovoltaics, more progress is needed in the detection/collection of light at low-level conditions. Traditional photodetectors tend to suffer from high noise when operated at room temperature; therefore, these devices require additional cooling systems to detect weak or dim light. Conventional solar cells also face the challenge of poor light-harvesting capabilities in hazy or cloudy weather. The real world features such varying levels of light, which makes it important to develop strategies that allow optical devices to function when conditions are less than optimal. In this work, we report an organic/inorganic hybrid device that consists of graphene quantum dot-modified poly(3,4-ethylenedioxythiophene) polystyrenesulfonate spin-coated on Si for the detection/harvest of weak light. The hybrid configuration provides the device with high responsivity and detectability, omnidirectional light trapping, and fast operation speed. To demonstrate the potential of this hybrid device in real world applications, we measured near-infrared light scattered through human tissue to demonstrate noninvasive oximetric photodetection as well as characterized the device\\'s photovoltaic properties in outdoor (i.e., weather-dependent) and indoor weak light conditions. This organic/inorganic device configuration demonstrates a promising strategy for developing future high-performance low-light compatible photodetectors and photovoltaics.
Hybrid spin and valley quantum computing with singlet-triplet qubits.
Rohling, Niklas; Russ, Maximilian; Burkard, Guido
2014-10-24
The valley degree of freedom in the electronic band structure of silicon, graphene, and other materials is often considered to be an obstacle for quantum computing (QC) based on electron spins in quantum dots. Here we show that control over the valley state opens new possibilities for quantum information processing. Combining qubits encoded in the singlet-triplet subspace of spin and valley states allows for universal QC using a universal two-qubit gate directly provided by the exchange interaction. We show how spin and valley qubits can be separated in order to allow for single-qubit rotations.
Quantum control of quasi-collision states: A protocol for hybrid fusion
Vilela Mendes, R.
2018-04-01
When confined to small regions quantum systems exhibit electronic and structural properties different from their free space behavior. These properties are of interest, for example, for molecular insertion, hydrogen storage and the exploration of new pathways for chemical and nuclear reactions. Here, a confined three-body problem is studied, with emphasis on the study of the “quantum scars” associated to dynamical collisions. For the particular case of nuclear reactions, it is proposed that a molecular cage might simply be used as a confining device with the collision states accessed by quantum control techniques.
Al-Khalili, Jim
2003-01-01
In this lively look at quantum science, a physicist takes you on an entertaining and enlightening journey through the basics of subatomic physics. Along the way, he examines the paradox of quantum mechanics--beautifully mathematical in theory but confoundingly unpredictable in the real world. Marvel at the Dual Slit experiment as a tiny atom passes through two separate openings at the same time. Ponder the peculiar communication of quantum particles, which can remain in touch no matter how far apart. Join the genius jewel thief as he carries out a quantum measurement on a diamond without ever touching the object in question. Baffle yourself with the bizzareness of quantum tunneling, the equivalent of traveling partway up a hill, only to disappear then reappear traveling down the opposite side. With its clean, colorful layout and conversational tone, this text will hook you into the conundrum that is quantum mechanics.
Quantum non-demolition phonon counter with a hybrid optomechnical system
Song, Qiao; Zhang, KeYe; Dong, Ying; Zhang, WeiPing
2018-05-01
A phonon counting scheme based on the control of polaritons in an optomechanical system is proposed. This approach permits us to measure the number of phonons in a quantum non-demolition (QND) manner for arbitrary modes not limited by the frequency matching condition as in usual photon-phonon scattering detections. The performance on phonon number transfer and quantum state transfer of the counter are analyzed and simulated numerically by taking into account all relevant sources of noise.
ZnO-nanocarbon core-shell type hybrid quantum dots
Choi, Won Kook
2017-01-01
This book offers a comprehensive overview of ZnO-nano carbon core shell hybrid issues. There is significant interest in metal oxide/nanocarbon hybrid functional materials in the field of energy conversion and storage as electrode materials for supercapacitors, Li ion secondary battery, electrocatalysts for water splitting, and optoelectronic devices such as light emitting diodes and solar photovoltaic cells. Despite efforts to manipulate more uniform metal oxide-nanocarbon nanocomposite structures, they have shown poor performance because they are randomly scattered and non-uniformly attached to the nanocarbon surface. For higher and more effective performance of the hybrid structure, 3D conformal coating on metal oxides are highly desirable. In the first part of the book, the physical and chemical properties of ZnO and nanocarbons and the state-of-the-art in related research are briefly summarized. In the next part, the 3D conformal coating synthetic processes of ZnO templated nanocarbon hybrid materials suc...
Lukashev, Eugeny P; Knox, Petr P; Gorokhov, Vladimir V; Grishanova, Nadezda P; Seifullina, Nuranija Kh; Krikunova, Maria; Lokstein, Heiko; Paschenko, Vladimir Z
2016-11-01
Quantum dots (QDs) absorb ultraviolet and long-wavelength visible light energy much more efficiently than natural bacterial light-harvesting proteins and can transfer the excitation energy to photosynthetic reaction centers (RCs). Inclusion of RCs combined with QDs as antennae into liposomes opens new opportunities for using such hybrid systems as a basis for artificial energy-transforming devices that potentially can operate with greater efficiency and stability than devices based only on biological components or inorganic components alone. RCs from Rhodobacter sphaeroides and QDs (CdSe/ZnS with hydrophilic covering) were embedded in lecithin liposomes by extrusion of a solution of multilayer lipid vesicles through a polycarbonate membrane or by dialysis of lipids and proteins dispersed with excess detergent. The efficiency of RC and QD interaction within the liposomes was estimated using fluorescence excitation spectra of the photoactive bacteriochlorophyll of the RCs and by measuring the fluorescence decay kinetics of the QDs. The functional activity of the RCs in hybrid complexes was fully maintained, and their stability was even increased. The efficiency of energy transfer between QDs and RCs and conditions of long-term stability of function of such hybrid complexes in film preparations were investigated as well. It was found that dry films containing RCs and QDs, maintained at atmospheric humidity, are capable of maintaining their functional activity for at least some months as judged by measurements of their spectral characteristics, efficiency of energy transfer from QDs to RCs and RC electron transport activity. Addition of trehalose to the films increases the stability further, especially for films maintained at low humidity. These stable hybrid film structures are promising for further studies towards developing new phototransformation devices for biotechnological applications. Copyright © 2016 Elsevier B.V. All rights reserved.
Tahvili, M.S.; Du, L.; Heck, M.J.R.; Nötzel, R.; Smit, M.K.; Bente, E.A.J.M.
2012-01-01
We present an investigation of passive and hybrid mode-locking in Fabry-Pérot type two-section InAs/InP(100) quantum dot lasers that show dual wavelength operation. Over the whole current and voltage range for mode-locking of these lasers, the optical output spectra show two distinct lobes. The two
Analysis of hybrid mode-locking of two-section quantum dot lasers operating at 1.5 μm
Heck, M.J.R.; Salumbides, E.J.; Renault, A.; Bente, E.A.J.M.; Oei, Y.S.; Smit, M.K.; Veldhoven, van P.J.; Nötzel, R.; Eikema, K.S.E.; Ubachs, W.
2009-01-01
For the first time a detailed study of hybrid mode-locking in two- section InAs/InP quantum dot Fabry-Pérot-type lasers is presented. The output pulses have a typical upchirp of approximately 8 ps/nm, leading to very elongated pulses. The mechanism leading to this typical pulse shape and the phase
Majorana bound states in a coupled quantum-dot hybrid-nanowire system
DEFF Research Database (Denmark)
Deng, M. T.; Vaitiekenas, S.; Hansen, E. B.
2016-01-01
Hybrid nanowires combining semiconductor and superconductor materials appear well suited for the creation, detection, and control of Majorana bound states (MBSs). We demonstrate the emergence of MBSs from coalescing Andreev bound states (ABSs) in a hybrid InAs nanowire with epitaxial Al, using...... with the end-dot bound state, which is in agreement with a numerical model. The ABS/MBS spectra provide parameters that are useful for understanding topological superconductivity in this system....
Wright, Joshua T.; Forsythe, Kyle; Hutchins, Jamie; Meulenberg, Robert W.
2016-04-01
This paper investigates how chemical dopants affect the electronic properties of CdSe quantum dots (QDs) and why a model that incorporates the concepts of orbital hybridization must be used to understand these properties. Extended X-ray absorption fine structure spectroscopy measurements show that copper dopants in CdSe QDs occur primarily through a statistical doping mechanism. Ultraviolet photoemission spectroscopy (UPS) experiments provide a detailed insight on the valence band (VB) structure of doped and undoped QDs. Using UPS measurements, we are able to observe photoemission from the Cu d-levels above VB maximum of the QDs which allows a complete picture of the energy band landscape of these materials. This information provides insights into many of the physical properties of doped QDs, including the highly debated near-infrared photoluminescence in Cu doped CdSe QDs. We show that all our results point to a common theme of orbital hybridization in Cu doped CdSe QDs which leads to optically and electronically active states below the conduction band minimum. Our model is supported from current-voltage measurements of doped and undoped materials, which exhibit Schottky to Ohmic behavior with Cu doping, suggestive of a tuning of the lowest energy states near the Fermi level.This paper investigates how chemical dopants affect the electronic properties of CdSe quantum dots (QDs) and why a model that incorporates the concepts of orbital hybridization must be used to understand these properties. Extended X-ray absorption fine structure spectroscopy measurements show that copper dopants in CdSe QDs occur primarily through a statistical doping mechanism. Ultraviolet photoemission spectroscopy (UPS) experiments provide a detailed insight on the valence band (VB) structure of doped and undoped QDs. Using UPS measurements, we are able to observe photoemission from the Cu d-levels above VB maximum of the QDs which allows a complete picture of the energy band landscape of
International Nuclear Information System (INIS)
Shin, Hyeondeok; Lee, Hoonkyung; Heinonen, Olle; Benali, Anouar; Kwon, Yongkyung
2017-01-01
α-graphyne is a two-dimensional sheet of sp-sp2 hybridized carbon atoms in a honeycomb lattice. While the geometrical structure is similar to that of graphene, the hybridized triple bonds give rise to electronic structure that is different from that of graphene. Similar to graphene, α-graphyne can be stacked in bilayers with two stable configurations, but the different stackings have very different electronic structures: one is predicted to have gapless parabolic bands and the other a tunable bandgap which is attractive for applications. In order to realize applications, it is crucial to understand which stacking is more stable. This is difficult to model, as the stability is a result of weak interlayer van der Waals interactions which are not well captured by density functional theory (DFT). We have used quantum Monte Carlo simulations that accurately include van der Waals interactions to calculate the interlayer binding energy of bilayer graphyne and to determine its most stable stacking mode. Our results show that inter-layer bindings of sp- and sp2-bonded carbon networks are significantly underestimated in a Kohn-Sham DFT approach, even with an exchange-correlation potential corrected to include, in some approximation, van der Waals interactions. Finally, our quantum Monte Carlo calculations reveal that the interlayer binding energy difference between the two stacking modes is only 0.9(4) eV/atom. From this we conclude that the two stable stacking modes of bilayer α-graphyne are almost degenerate with each other, and both will occur with about the same probability at room temperature unless there is a synthesis path that prefers one stacking over the other.
Wang, Le; Zong, Shenfei; Wang, Zhuyuan; Lu, Ju; Chen, Chen; Zhang, Ruohu; Cui, Yiping
2018-07-13
Single molecule localization microscopy (SMLM) is a powerful tool for imaging biological targets at the nanoscale. In this report, we present SMLM imaging of telomeres and centromeres using fluorescence in situ hybridization (FISH). The FISH probes were fabricated by decorating CdSSe/ZnS quantum dots (QDs) with telomere or centromere complementary DNA strands. SMLM imaging experiments using commercially available peptide nucleic acid (PNA) probes labeled with organic fluorophores were also conducted to demonstrate the advantages of using QDs FISH probes. Compared with the PNA probes, the QDs probes have the following merits. First, the fluorescence blinking of QDs can be realized in aqueous solution or PBS buffer without thiol, which is a key buffer component for organic fluorophores' blinking. Second, fluorescence blinking of the QDs probe needs only one excitation light (i.e. 405 nm). While fluorescence blinking of the organic fluorophores usually requires two illumination lights, that is, the activation light (i.e. 405 nm) and the imaging light. Third, the high quantum yield, multiple switching times and a good optical stability make the QDs more suitable for long-term imaging. The localization precision achieved in telomeres and centromeres imaging experiments is about 30 nm, which is far beyond the diffraction limit. SMLM has enabled new insights into telomeres or centromeres on the molecular level, and it is even possible to determine the length of telomere and become a potential technique for telomere-related investigation.
Tavares, Anthony J; Noor, M Omair; Vannoy, Charles H; Algar, W Russ; Krull, Ulrich J
2012-01-03
The glass surface of a glass-polydimethylsiloxane (PDMS) microfluidic channel was modified to develop a solid-phase assay for quantitative determination of nucleic acids. Electroosmotic flow (EOF) within channels was used to deliver and immobilize semiconductor quantum dots (QDs), and electrophoresis was used to decorate the QDs with oligonucleotide probe sequences. These processes took only minutes to complete. The QDs served as energy donors in fluorescence resonance energy transfer (FRET) for transduction of nucleic acid hybridization. Electrokinetic injection of fluorescent dye (Cy3) labeled oligonucleotide target into a microfluidic channel and subsequent hybridization (within minutes) provided the proximity for FRET, with emission from Cy3 being the analytical signal. The quantification of target concentration was achieved by measurement of the spatial length of coverage by target along a channel. Detection of femtomole quantities of target was possible with a dynamic range spanning an order of magnitude. The assay provided excellent resistance to nonspecific interactions of DNA. Further selectivity of the assay was achieved using 20% formamide, which allowed discrimination between a fully complementary target and a 3 base pair mismatch target at a contrast ratio of 4:1. © 2011 American Chemical Society
Energy Technology Data Exchange (ETDEWEB)
Wright, Joshua T.; Forsythe, Kyle; Hutchins, Jamie; Meulenberg, Robert W.
2016-04-13
This paper investigates how chemical dopants affect the electronic properties of CdSe quantum dots (QDs) and why a model that incorporates the concepts of orbital hybridization must be used to understand these properties. Extended X-ray absorption fine structure spectroscopy measurements show that copper dopants in CdSe QDs occur primarily through a statistical doping mechanism. Ultraviolet photoemission spectroscopy (UPS) experiments provide a detailed insight on the valence band (VB) structure of doped and undoped QDs. Using UPS measurements, we are able to observe photoemission from the Cu d-levels above VB maximum of the QDs which allows a complete picture of the energy band landscape of these materials. This information provides insights into many of the physical properties of doped QDs, including the highly debated near-infrared photoluminescence in Cu doped CdSe QDs. We show that all our results point to a common theme of orbital hybridization in Cu doped CdSe QDs which leads to optically and electronically active states below the conduction band minimum. Our model is supported from current–voltage measurements of doped and undoped materials, which exhibit Schottky to Ohmic behavior with Cu doping, suggestive of a tuning of the lowest energy states near the Fermi level.
Hybrid GaAs/AlGaAs Nanowire—Quantum dot System for Single Photon Sources
DEFF Research Database (Denmark)
Cirlin, G.; Reznik, R.; Shtrom, I.
2018-01-01
III–V nanowires, or a combination of the nanowires with quantum dots, are promising building blocks for future optoelectronic devices, in particular, single-photon emitters, lasers and photodetectors. In this work we present results of molecular beam epitaxial growth of combined nanostructures...
Application of Inkjet Printing in High-Density Pixelated RGB Quantum Dot-Hybrid LEDs
Haverinen, Hanna; Jabbour, Ghassan E.
2012-01-01
to fabricate high-density, pixelated (quarter video graphics array (QVGA) format), monochromatic and RGB quantum dots light-emitting diodes (QDLEDs), where inkjet printing is used to deposit the light-emitting layer of QDs. It shows some of the factors
Improved Green’s function measurement for hybridization expansion quantum Monte Carlo
Czech Academy of Sciences Publication Activity Database
Augustinský, Pavel; Kuneš, Jan
2013-01-01
Roč. 184, č. 9 (2013), s. 2119-2126 ISSN 0010-4655 Institutional support: RVO:68378271 Keywords : continuous time quantum Monte Carlo method * Green function estimator Subject RIV: BE - Theoretical Physics Impact factor: 2.407, year: 2013
Hybrid Optical-Magnetic Traps for Studies of 2D Quantum Turbulence in Bose-Einstein Condensates
Myers, Jessica Ann
Turbulence appears in most natural and man-made flows. However, the analysis of turbulence is particularly difficult. Links between microscopic fluid dynamics and statistical signatures of turbulence appear unobtainable from the postulates of fluid dynamics making turbulence one of the most important unsolved theoretical problems in physics. Two-dimensional quantum turbulence (2DQT), an emerging field of study, involves turbulence in two-dimensional (2D) flows in superfluids, such as Bose-Einstein condensates (BECs). In 2D superfluids, a turbulent state can be characterized by a disordered distribution of numerous vortex cores. The question of how to effectively and efficiently generate turbulent states in superfluids is a fundamental question in the field of quantum turbulence. Therefore, experimental studies of vortex nucleation and the onset of turbulence in a superfluid are important for achieving a deeper understanding of the overall problem of turbulence. My PhD dissertation involves the study of vortex nucleation and the onset of turbulence in quasi-2D BECs. First, I discuss experimental apparatus advancements that now enable BECs to be created in a hybrid optical-magnetic trap, an atom trapping configuration conducive to 2DQT experiments. Next, I discuss the design and construction of a quantum vortex microscope and initial vortex detection tests. Finally, I present the first experiments aimed at studying 2DQT carried out in the updated apparatus. Thermal counterflow in superfluid helium, in which the normal and superfluid components flow in opposite directions, is known to create turbulence in the superfluid. However, this phenomenon has not been simulated or studied in dilute-gas BECs as a possible vortex nucleation method. In this dissertation, I present preliminary data from the first experiments aimed at understanding thermal counterflow turbulence in dilute-gas BECs.
The top-transmon: a hybrid superconducting qubit for parity-protected quantum computation
International Nuclear Information System (INIS)
Hassler, F; Akhmerov, A R; Beenakker, C W J
2011-01-01
Qubits constructed from uncoupled Majorana fermions are protected from decoherence, but to perform a quantum computation this topological protection needs to be broken. Parity-protected quantum computation breaks the protection in a minimally invasive way, by coupling directly to the fermion parity of the system-irrespective of any quasiparticle excitations. Here, we propose to use a superconducting charge qubit in a transmission line resonator (the so-called transmon) to perform parity-protected rotations and read-out of a topological (top) qubit. The advantage over an earlier proposal using a flux qubit is that the coupling can be switched on and off with exponential accuracy, promising a reduced sensitivity to charge noise.
Application of Inkjet Printing in High-Density Pixelated RGB Quantum Dot-Hybrid LEDs
Haverinen, Hanna
2012-05-23
Recently, an intriguing solution to obtain better color purity has been to introduce inorganic emissive quantum dots (QDs) into an otherwise OLED structure. The emphasis of this chapter is to present a simple discussion of the first attempts to fabricate high-density, pixelated (quarter video graphics array (QVGA) format), monochromatic and RGB quantum dots light-emitting diodes (QDLEDs), where inkjet printing is used to deposit the light-emitting layer of QDs. It shows some of the factors that have to be considered in order to achieve the desired accuracy and printing quality. The successful operation of the RGB printed devices indicates the potential of the inkjet printing approach in the fabrication of full-color QDLEDs for display application. However, further optimization of print quality is still needed in order to eliminate the formation of pinholes, thus maximizing energy transfer from organic layers to the QDs and in turn increasing the performance of the devices. Controlled Vocabulary Terms: ink jet printing; LED displays; LED lamps; organic light emitting diodes; quantum dots
Surface plasmon enhanced quantum transport in a hybrid metal nanoparticle array
International Nuclear Information System (INIS)
Sun, Lin; Nan, Yali; Xu, Shang; Zhang, Sishi; Han, Min
2014-01-01
Hybrid Pd–Ag nanoparticle arrays composed of randomly distributed Pd nanoparticles in dense packing and a small number of dispersed Ag nanoparticles were fabricated with controlled coverage. Photo-enhanced conductance was observed in the nanoparticle arrays. Largest enhancement, which can be higher than 20 folds, was obtained with 450 nm light illumination. This wavelength was found to correlate with the surface plasmon resonance of the Ag nanoparticles. Electron transport measurements showed there were significant Coulomb blockade in the nanoparticle arrays and the blockade could be overcome with the surface plasmon enhanced local field of Ag nanoparticles induced by light illumination. - Highlights: • We study photo-enhanced electron conductance of a hybrid Pd–Ag nanoparticle array. • The light-induced conductance enhancement is as high as 20 folds at 10 K. • The enhancement is correlate with the surface plasmon resonance of Ag nanoparticles. • Coulomb blockades is overcome with the surface plasmon enhanced local field
Microcanonical and hybrid simulations of lattice quantum chromodynamics with dynamical fermions
International Nuclear Information System (INIS)
Sinclair, D.K.
1986-10-01
Lattice QCD is simulated using Microcanonical and Hybrid (Micro-canonical/Langevin) methods to facilitate the inclusion of dynamical fermions (quarks). We report on simulations with 4 flavors of light dynamical quarks on a 10 3 x 6 lattice to study the finite temperature deconfinement/chiral transition which should be observable in relativistic heavy ion collisions, as a function of quark mass. A first order transition is observed at large mass, weakens at intermediate mass and strengthens for very small quark mass
Quantum confinement of zero-dimensional hybrid organic-inorganic polaritons at room temperature
Nguyen, H. S.; Han, Z.; Abdel-Baki, K.; Lafosse, X.; Amo, A.; Lauret, J.-S.; Deleporte, E.; Bouchoule, S.; Bloch, J.
2014-02-01
We report on the quantum confinement of zero-dimensional polaritons in perovskite-based microcavity at room temperature. Photoluminescence of discrete polaritonic states is observed for polaritons localized in symmetric sphere-like defects which are spontaneously nucleated on the top dielectric Bragg mirror. The linewidth of these confined states is found much sharper (almost one order of magnitude) than that of photonic modes in the perovskite planar microcavity. Our results show the possibility to study organic-inorganic cavity polaritons in confined microstructure and suggest a fabrication method to realize integrated polaritonic devices operating at room temperature.
Quantum confinement of zero-dimensional hybrid organic-inorganic polaritons at room temperature
International Nuclear Information System (INIS)
Nguyen, H. S.; Lafosse, X.; Amo, A.; Bouchoule, S.; Bloch, J.; Han, Z.; Abdel-Baki, K.; Lauret, J.-S.; Deleporte, E.
2014-01-01
We report on the quantum confinement of zero-dimensional polaritons in perovskite-based microcavity at room temperature. Photoluminescence of discrete polaritonic states is observed for polaritons localized in symmetric sphere-like defects which are spontaneously nucleated on the top dielectric Bragg mirror. The linewidth of these confined states is found much sharper (almost one order of magnitude) than that of photonic modes in the perovskite planar microcavity. Our results show the possibility to study organic-inorganic cavity polaritons in confined microstructure and suggest a fabrication method to realize integrated polaritonic devices operating at room temperature
Enhanced performance of hybrid solar cells using longer arms of quantum cadmium selenide tetrapods
Lee, Kyu-Sung
2011-12-01
We demonstrate that enhanced device performance of hybrid solar cells based on tetrapod (TP)-shaped cadmium selenide (CdSe) nanoparticles and conjugated polymer of poly (3-hexylthiophene) (P3HT) can be obtained by using longer armed tetrapods which aids in better spatial connectivity, thus decreasing charge hopping events which lead to better charge transport. Longer tetrapods with 10 nm arm length lead to improved power conversion efficiency of 1.12% compared to 0.80% of device having 5 nm short-armed tetrapods:P3HT photoactive blends.
Enhanced performance of hybrid solar cells using longer arms of quantum cadmium selenide tetrapods
Lee, Kyu-Sung; Kim, Inho; Gullapalli, Sravani; Wong, Michael S.; Jabbour, Ghassan E.
2011-01-01
We demonstrate that enhanced device performance of hybrid solar cells based on tetrapod (TP)-shaped cadmium selenide (CdSe) nanoparticles and conjugated polymer of poly (3-hexylthiophene) (P3HT) can be obtained by using longer armed tetrapods which aids in better spatial connectivity, thus decreasing charge hopping events which lead to better charge transport. Longer tetrapods with 10 nm arm length lead to improved power conversion efficiency of 1.12% compared to 0.80% of device having 5 nm short-armed tetrapods:P3HT photoactive blends.
Döntgen, Malte; Schmalz, Felix; Kopp, Wassja A; Kröger, Leif C; Leonhard, Kai
2018-06-13
An automated scheme for obtaining chemical kinetic models from scratch using reactive molecular dynamics and quantum chemistry simulations is presented. This methodology combines the phase space sampling of reactive molecular dynamics with the thermochemistry and kinetics prediction capabilities of quantum mechanics. This scheme provides the NASA polynomial and modified Arrhenius equation parameters for all species and reactions that are observed during the simulation and supplies them in the ChemKin format. The ab initio level of theory for predictions is easily exchangeable and the presently used G3MP2 level of theory is found to reliably reproduce hydrogen and methane oxidation thermochemistry and kinetics data. Chemical kinetic models obtained with this approach are ready-to-use for, e.g., ignition delay time simulations, as shown for hydrogen combustion. The presented extension of the ChemTraYzer approach can be used as a basis for methodologically advancing chemical kinetic modeling schemes and as a black-box approach to generate chemical kinetic models.
Rangel-Mendez, Jose R.; Matos, Juan; Cházaro-Ruiz, Luis F.; González-Castillo, Ana C.; Barrios-Yáñez, Guillermo
2018-03-01
The microwave-assisted solvothermal synthesis of C-doped TiO2 and ZnO hybrid materials was performed. Saccharose, titanium isopropoxide and zinc acetate were used as organic and inorganic sources for the synthesis. The influence of temperature and reaction time on the textural and optoelectronic properties of the hybrid materials was verified. Carbon quantum-dots of TiO2 and ZnO nanostructured spheres were obtained in a second pot by controlled calcination steps of the precursor hybrid materials. A carefully characterization by adsorption-desorption N2 isotherms, XRD, XPS, SEM, UV-vis/DR and electro- and photo-electrochemistry properties of the carbon quantum-dots TiO2 and ZnO spheres was performed. The photoelectrochemical activity of TiO2-C and ZnO-C films proved to be dependent on the conditions of synthesis. It was found a red-shift in the energy band gap of the semiconductors with values of 3.02 eV and 3.13 eV for the TiO2-C and ZnO-C, respectively, clearly lower than those on bare semiconductors, which is associated with the C-doping effect. From the photo-electrochemistry characterization of C-doped TiO2 and ZnO films can be concluded that the present materials have potential applications as photoelectrodes for quantum-dots sensitized solar cells.
Algar, W Russ; Krull, Ulrich J
2010-01-01
A multiplexed solid-phase assay for the detection of nucleic acid hybridization was developed on the basis of a single color of immobilized CdSe/ZnS quantum dot (QD) as a donor in fluorescence resonance energy transfer (FRET). This work demonstrated that two channels of detection did not necessitate two different QD donors. Two probe oligonucleotides were coimmobilized on optical fibers modified with QDs, and a sandwich assay was used to associate the acceptor dyes with interfacial hybridization events without target labeling. FRET-sensitized acceptor emission provided an analytical signal that was concentration dependent down to 10 nM. Changes in the ratio of coimmobilized probe oligonucleotides were found to yield linear changes in the relative amounts of acceptor emission. These changes were compared to previous studies that used mixed films of two QD donors for two detection channels. The analysis indicated that probe dilution effects were primarily driven by changes in acceptor number density and that QD dilution effects or changes in mean donor-acceptor distance were secondary. Hybridization kinetics were found to be consistent between different ratios of coimmobilized probes, suggesting that hybridization in this type of system occurred via the accepted model for solid-phase hybridization, where adsorption and then diffusion at the solid interface drove hybridization.
Energy Technology Data Exchange (ETDEWEB)
Lv, Ouyang; Tao, Yongxin; Qin, Yong [Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou 213164 (China); Chen, Chuanxiang [School of Environmental and Chemical Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003 (China); Pan, Yan; Deng, Linhong [Institute of Biomedical Engineering and Health Sciences, Changzhou University, Changzhou 213164 (China); Liu, Li [School of pharmaceutical Engineering & Life Science, Changzhou University, Changzhou 213164 (China); Kong, Yong, E-mail: yzkongyong@126.com [Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, School of Petrochemical Engineering, Changzhou University, Changzhou 213164 (China)
2016-10-01
Highly fluorescent graphene quantum dots (GQDs)-chitosan (CS) hybrid xerogels (GQDs-CS) were facilely synthesized, and the morphology of GQDs-CS was controllable by varying the content of GQDs in the xerogel. The GQDs-CS exhibited a porous and three-dimensional (3D) network structure when the content of GQDs reached 43% (wt%) in the xerogel, which was beneficial for drug loading and sustained release. The as-prepared GQDs-CS could also be applied for in vivo imaging since it showed strong blue, green and red luminescence under excitation of varying wavelengths. Moreover, the pH-induced protonation/deprotonation of the –NH{sub 2} groups on CS chains can result in a pH-dependent drug delivery behavior of the GQDs-CS hybrid xerogel. - Graphical abstract: Highly fluorescent and morphology-controllable graphene quantum dots-chitosan hybrid xerogels for in vivo imaging and pH-sensitive drug carrier. Display Omitted - Highlights: • Highly fluorescent GQDs-CS hybrid xerogels were facilely synthesized. • The as-made xerogels exhibited various morphologies with different GQDs contents. • The GQDs-CS exhibited a porous and 3D network when the content of GQDs reached 43%. • The GQDs-CS could be applied for in vivo imaging since it showed strong luminescence. • The protonation/deprotonation of –NH{sub 2} on CS result in a pH-dependent drug delivery.
International Nuclear Information System (INIS)
Lv, Ouyang; Tao, Yongxin; Qin, Yong; Chen, Chuanxiang; Pan, Yan; Deng, Linhong; Liu, Li; Kong, Yong
2016-01-01
Highly fluorescent graphene quantum dots (GQDs)-chitosan (CS) hybrid xerogels (GQDs-CS) were facilely synthesized, and the morphology of GQDs-CS was controllable by varying the content of GQDs in the xerogel. The GQDs-CS exhibited a porous and three-dimensional (3D) network structure when the content of GQDs reached 43% (wt%) in the xerogel, which was beneficial for drug loading and sustained release. The as-prepared GQDs-CS could also be applied for in vivo imaging since it showed strong blue, green and red luminescence under excitation of varying wavelengths. Moreover, the pH-induced protonation/deprotonation of the –NH_2 groups on CS chains can result in a pH-dependent drug delivery behavior of the GQDs-CS hybrid xerogel. - Graphical abstract: Highly fluorescent and morphology-controllable graphene quantum dots-chitosan hybrid xerogels for in vivo imaging and pH-sensitive drug carrier. Display Omitted - Highlights: • Highly fluorescent GQDs-CS hybrid xerogels were facilely synthesized. • The as-made xerogels exhibited various morphologies with different GQDs contents. • The GQDs-CS exhibited a porous and 3D network when the content of GQDs reached 43%. • The GQDs-CS could be applied for in vivo imaging since it showed strong luminescence. • The protonation/deprotonation of –NH_2 on CS result in a pH-dependent drug delivery.
Lim, Hwain; Lee, Kyu Seung; Liu, Yang; Kim, Hak Yong; Son, Dong Ick
2018-05-01
We report the synthesis and characterization of the carbon quantum dots (C-dots) easily obtained from citric acid and ethanediamine, and also investigated structural, optical and electrical properties. The C-dots have extraordinary optical and electrical features such as absorption of ultraviolet range and effective interface for charge separation and transport in active layer, which make them attractive materials for applications in photovoltaic devices (PV). The C-dots play important roles in charge extraction in the PV structures, they can be synthesized by a simple method and used to insert in active layer of polymer solar cells. In this study, we demonstrate that improve charge transport properties of inverted polymer solar cells (iPSCs) with C-dots and structural, optical and electrical properties of C-dots. As a result, iPSCs with C-dots showed enhancement of more than 30% compared with that of the contrast device in power conversion efficiency.
Tunable hybridization of Majorana bound states at the quantum spin Hall edge
Keidel, Felix; Burset, Pablo; Trauzettel, Björn
2018-02-01
Confinement at the helical edge of a topological insulator is possible in the presence of proximity-induced magnetic (F) or superconducting (S) order. The interplay of both phenomena leads to the formation of localized Majorana bound states (MBS) or likewise (under certain resonance conditions) the formation of ordinary Andreev bound states (ABS). We investigate the properties of bound states in junctions composed of alternating regions of F or S barriers. Interestingly, the direction of magnetization in F regions and the relative superconducting phase between S regions can be exploited to hybridize MBS or ABS at will. We show that the local properties of MBS translate into a particular nonlocal superconducting pairing amplitude. Remarkably, the symmetry of the pairing amplitude contains information about the nature of the bound state that it stems from. Hence this symmetry can in principle be used to distinguish MBS from ABS, owing to the strong connection between local density of states and nonlocal pairing in our setup.
Sun, Mingye; Zheng, Youjin; Zhang, Lei; Zhao, Liping; Zhang, Bing
2017-08-01
The influence of heat treatment on hole transfer (HT) processes from the CdSe/ZnS and CdSe/CdS/ZnS quantum dots (QDs) to 4,4‧,4″-Tris(carbazol-9-yl)-triphenylamine (TCTA) in QD/TCTA hybrid films has been researched with time-resolved photoluminescence (PL) spectroscopy. The PL dynamic results demonstrated a heat-treatment-temperature-dependent HT process from the core-shell CdSe QDs to TCTA. The HT rates and efficiencies can be effectively increased due to reduced distance between core-shell CdSe QDs and TCTA after heat treatment. The CdS shell exhibited a more obvious effect on HT from the core-shell CdSe QDs to TCTA than on electron transfer to TiO2, due to higher barrier for holes to tunnel through CdS shell and larger effective mass of holes in CdS than electrons. These results indicate that heat treatment would be an effective means to further optimize solid-state QD sensitized solar cells and rational design of CdS shell is significant.
Ryckaert, Jana; Correia, António; Tessier, Mickael D; Dupont, Dorian; Hens, Zeger; Hanselaer, Peter; Meuret, Youri
2017-11-27
Quantum dots can be used in white LEDs for lighting applications to fill the spectral gaps in the combined emission spectrum of the blue pumping LED and a broad band phosphor, in order to improve the source color rendering properties. Because quantum dots are low scattering materials, their use can also reduce the amount of backscattered light which can increase the overall efficiency of the white LED. The absorption spectrum and narrow emission spectrum of quantum dots can be easily tuned by altering their synthesis parameters. Due to the re-absorption events between the different luminescent materials and the light interaction with the LED package, determining the optimal quantum dot properties is a highly non-trivial task. In this paper we propose a methodology to select the optimal quantum dot to be combined with a broad band phosphor in order to realize a white LED with optimal luminous efficacy and CRI. The methodology is based on accurate and efficient simulations using the extended adding-doubling approach that take into account all the optical interactions. The method is elaborated for the specific case of a hybrid, remote phosphor white LED with YAG:Ce phosphor in combination with InP/CdxZn 1-x Se type quantum dots. The absorption and emission spectrum of the quantum dots are generated in function of three synthesis parameters (core size, shell size and cadmium fraction) by a semi-empirical 'quantum dot model' to include the continuous tunability of these spectra. The sufficiently fast simulations allow to scan the full parameter space consisting of these synthesis parameters and luminescent material concentrations in terms of CRI and efficacy. A conclusive visualization of the final performance allows to make a well-considered trade-off between these performance parameters. For the hybrid white remote phosphor LED with YAG:Ce and InP/CdxZn 1-x Se quantum dots a CRI Ra = 90 (with R9>50) and an overall efficacy of 110 lm/W is found.
A novel quantum dot-laccase hybrid nanobiosensor for low level determination of dopamine.
Shamsipur, Mojtaba; Shanehasz, Maryam; Khajeh, Khosro; Mollania, Nasrin; Kazemi, Sayyed Habib
2012-12-07
This work reports a novel nanobiosensor based on a thioglycolic acid (TGA)-capped CdTe quantum dot-laccase (Lac) enzyme system for sensitive detection of dopamine (DA). The enzyme used catalyzes the oxidation of DA to dopamine-o-quinone (DOQ), which can selectively quench the strong luminescence of CdTe nanocrystals at neutral pH. The relationship between luminescence intensity of CdTe nanocrystals and DA concentration is nicely described by the Stern-Volmer equation. At an optimum pH of 7.4, the proposed sensor gives a linear calibration over a DA concentration range of 0.3 to 100 μM, with a limit of detection of 0.16 μM and a response time of 2 min. The relative standard deviation for seven replicate determinations of 6.0 μM of DA was found to be 3.7%. The sensor was successfully applied to the determination of DA in a blood plasma sample and in a DA injection formulation.
Hybrid organic–inorganic inks flatten the energy landscape in colloidal quantum dot solids
Liu, Mengxia
2016-11-14
Bandtail states in disordered semiconductor materials result in losses in open-circuit voltage (Voc) and inhibit carrier transport in photovoltaics. For colloidal quantum dot (CQD) films that promise low-cost, large-area, air-stable photovoltaics, bandtails are determined by CQD synthetic polydispersity and inhomogeneous aggregation during the ligand-exchange process. Here we introduce a new method for the synthesis of solution-phase ligand-exchanged CQD inks that enable a flat energy landscape and an advantageously high packing density. In the solid state, these materials exhibit a sharper bandtail and reduced energy funnelling compared with the previous best CQD thin films for photovoltaics. Consequently, we demonstrate solar cells with higher Voc and more efficient charge injection into the electron acceptor, allowing the use of a closer-to-optimum bandgap to absorb more light. These enable the fabrication of CQD solar cells made via a solution-phase ligand exchange, with a certified power conversion efficiency of 11.28%. The devices are stable when stored in air, unencapsulated, for over 1,000 h.
Hybrid organic–inorganic inks flatten the energy landscape in colloidal quantum dot solids
Liu, Mengxia; Voznyy, Oleksandr; Sabatini, Randy; Arquer, F. Pelayo Garcí a de; Munir, Rahim; Balawi, Ahmed Hesham; Lan, Xinzheng; Fan, Fengjia; Walters, Grant; Kirmani, Ahmad R.; Hoogland, Sjoerd; Laquai, Fré dé ric; Amassian, Aram; Sargent, Edward H.
2016-01-01
Bandtail states in disordered semiconductor materials result in losses in open-circuit voltage (Voc) and inhibit carrier transport in photovoltaics. For colloidal quantum dot (CQD) films that promise low-cost, large-area, air-stable photovoltaics, bandtails are determined by CQD synthetic polydispersity and inhomogeneous aggregation during the ligand-exchange process. Here we introduce a new method for the synthesis of solution-phase ligand-exchanged CQD inks that enable a flat energy landscape and an advantageously high packing density. In the solid state, these materials exhibit a sharper bandtail and reduced energy funnelling compared with the previous best CQD thin films for photovoltaics. Consequently, we demonstrate solar cells with higher Voc and more efficient charge injection into the electron acceptor, allowing the use of a closer-to-optimum bandgap to absorb more light. These enable the fabrication of CQD solar cells made via a solution-phase ligand exchange, with a certified power conversion efficiency of 11.28%. The devices are stable when stored in air, unencapsulated, for over 1,000 h.
Long, Run; Prezhdo, Oleg V
2015-07-08
Hybrid organic/inorganic polymer/quantum dot (QD) solar cells are an attractive alternative to the traditional cells. The original, simple models postulate that one-dimensional polymers have continuous energy levels, while zero-dimensional QDs exhibit atom-like electronic structure. A realistic, atomistic viewpoint provides an alternative description. Electronic states in polymers are molecule-like: finite in size and discrete in energy. QDs are composed of many atoms and have high, bulk-like densities of states. We employ ab initio time-domain simulation to model the experimentally observed ultrafast photoinduced dynamics in a QD/polymer hybrid and show that an atomistic description is essential for understanding the time-resolved experimental data. Both electron and hole transfers across the interface exhibit subpicosecond time scales. The interfacial processes are fast due to strong electronic donor-acceptor, as evidenced by the densities of the photoexcited states which are delocalized between the donor and the acceptor. The nonadiabatic charge-phonon coupling is also strong, especially in the polymer, resulting in rapid energy losses. The electron transfer from the polymer is notably faster than the hole transfer from the QD, due to a significantly higher density of acceptor states. The stronger molecule-like electronic and charge-phonon coupling in the polymer rationalizes why the electron-hole recombination inside the polymer is several orders of magnitude faster than in the QD. As a result, experiments exhibit multiple transfer times for the long-lived hole inside the QD, ranging from subpicoseconds to nanoseconds. In contrast, transfer of the short-lived electron inside the polymer does not occur beyond the first picosecond. The energy lost by the hole on its transit into the polymer is accommodated by polymer's high-frequency vibrations. The energy lost by the electron injected into the QD is accommodated primarily by much lower-frequency collective and
Raksawong, Phannika; Chullasat, Kochaporn; Nurerk, Piyaluk; Kanatharana, Proespichaya; Davis, Frank; Bunkoed, Opas
2017-08-01
A hybrid molecularly imprinted polymer (MIP)-coated quantum dot (QD) nanocomposite was synthesized and applied as a fluorescence probe for the highly sensitive and selective determination of salbutamol. The hybrid MIP-coated QD nanocomposite was synthesized via a copolymerization process in the presence of thioglycolic acid capped CdTe QDs with salbutamol as a template, 3-aminopropyltriethoxysilane as the functional monomer, and tetraethyl orthosilicate as a cross-linker. The optimum molar ratio of template, monomer, and cross-linker was 1:6:20. The fluorescence intensity of the hybrid MIP-coated QDs was efficiently quenched after salbutamol rebound to the recognition sites, as a result of charge transfer from QDs to salbutamol. The synthesized hybrid MIP-coated QD nanocomposite showed high sensitivity and good selectivity toward salbutamol. Under the optimal recognition conditions, the fluorescence intensity was quenched linearly with increasing concentration of salbutamol in the range from 0.10 to 25.0 μg L -1 , with a detection limit of 0.034 μg L -1 . The hybrid optosensor developed was successfully applied in the determination of salbutamol in animal feeds and meat samples. Satisfactory recoveries were obtained in the range from 85% to 98%, with a standard deviation of less than 8%. Furthermore, the accuracy of the hybrid MIP-coated QD nanocomposite was investigated by comparison with a conventional high-performance liquid chromatography method, with the results obtained with two methods agreeing well with each other. The advantages of this sensing method are simplicity, rapidity, cost-effectiveness, high sensitivity, and good selectivity. Graphical Abstract The synthesis of hybrid MIP-coated QDs nanocomposite.
Noor, M Omair; Shahmuradyan, Anna; Krull, Ulrich J
2013-02-05
A paper-based solid-phase assay is presented for transduction of nucleic acid hybridization using immobilized quantum dots (QDs) as donors in fluorescence resonance energy transfer (FRET). The surface of paper was modified with imidazole groups to immobilize QD-probe oligonucleotide conjugates that were assembled in solution. Green-emitting QDs (gQDs) were FRET-paired with Cy3 acceptor. Hybridization of Cy3-labeled oligonucleotide targets provided the proximity required for FRET-sensitized emission from Cy3, which served as an analytical signal. The assay exhibited rapid transduction of nucleic acid hybridization within minutes. Without any amplification steps, the limit of detection of the assay was found to be 300 fmol with the upper limit of the dynamic range at 5 pmol. The implementation of glutathione-coated QDs for the development of nucleic acid hybridization assay integrated on a paper-based platform exhibited excellent resistance to nonspecific adsorption of oligonucleotides and showed no reduction in the performance of the assay in the presence of large quantities of noncomplementary DNA. The selectivity of nucleic acid hybridization was demonstrated by single-nucleotide polymorphism (SNP) detection at a contrast ratio of 19 to 1. The reuse of paper over multiple cycles of hybridization and dehybridization was possible, with less than 20% reduction in the performance of the assay in five cycles. This work provides an important framework for the development of paper-based solid-phase QD-FRET nucleic acid hybridization assays that make use of a ratiometric approach for detection and analysis.
Development and new applications of quantum chemical simulation methodology
International Nuclear Information System (INIS)
Weiss, A. K. H.
2012-01-01
The Division of Theoretical Chemistry at the University of Innsbruck is focused on the study of chemical compounds in aqueous solution, in terms of mainly hybrid quantum mechanical / molecular mechanical molecular dynamics simulations (QM/MM MD). Besides the standard means of data analysis employed for such simulations, this study presents several advanced and capable algorithms for the description of structural and dynamic properties of the simulated species and its hydration. The first part of this thesis further presents selected exemplary simulations, in particular a comparative study of Formamide and N-methylformamide, Guanidinium, and Urea. An included review article further summarizes the major advances of these studies. The computer programs developed in the course of this thesis are by now well established in the research field. The second part of this study presents the theory and a development guide for a quantum chemical program, QuMuLuS, that is by now used as a QM program for recent QM/MM simulations at the division. In its course, this part presents newly developed algorithms for electron integral evaluation and point charge embedding. This program is validated in terms of benchmark computations. The associated theory is presented on a detailed level, to serve as a source for contemporary and future studies in the division. In the third and final part, further investigations of related topics are addressed. This covers additional schemes of molecular simulation analysis, new software, as well as a mathematical investigation of a non-standard two-electron integral. (author)
Sapori, Daniel; Kepenekian, Mikaël; Pedesseau, Laurent; Katan, Claudine; Even, Jacky
2016-03-01
Quantum confinement as well as high frequency ε∞ and static εs dielectric profiles are described for nanoplatelets of halide inorganic perovskites CsPbX3 (X = I, Br, Cl) and hybrid organic-inorganic perovskites (HOP) in two-dimensional (2D) and three-dimensional (3D) structures. 3D HOP are currently being sought for their impressive photovoltaic ability. Prior to this sudden popularity, 2D HOP materials were driving intense activity in the field of optoelectronics. Such developments have been enriched by the recent ability to synthesize colloidal nanostructures of controlled sizes of 2D and 3D HOP. This raises the need to achieve a thorough description of the electronic structure and dielectric properties of these systems. In this work, we go beyond the abrupt dielectric interface model and reach the atomic scale description. We examine the influence of the nature of the halogen and of the cation on the band structure and dielectric constants. Similarly, we survey the effect of dimensionality and shape of the perovskite. In agreement with recent experimental results, we show an increase of the band gap and a decrease of ε∞ when the size of a nanoplatelet reduces. By inspecting 2D HOP, we find that it cannot be described as a simple superposition of independent inorganic and organic layers. Finally, the dramatic impact of ionic contributions on the dielectric constant εs is analysed.Quantum confinement as well as high frequency ε∞ and static εs dielectric profiles are described for nanoplatelets of halide inorganic perovskites CsPbX3 (X = I, Br, Cl) and hybrid organic-inorganic perovskites (HOP) in two-dimensional (2D) and three-dimensional (3D) structures. 3D HOP are currently being sought for their impressive photovoltaic ability. Prior to this sudden popularity, 2D HOP materials were driving intense activity in the field of optoelectronics. Such developments have been enriched by the recent ability to synthesize colloidal nanostructures of controlled
Energy Technology Data Exchange (ETDEWEB)
Hmar, Jehova Jire L.; Majumder, Tanmoy; Dhar, Saurab; Mondal, Suvra Prakash, E-mail: suvraphy@gmail.com
2016-08-01
S and N co-doped graphene quantum dots (S,N-GQDs) have been synthesized by a hydrothermal process. S,N-GQDs are made up of 1–5 monolayer of graphene with average diameter 13.3 nm. The absorption peaks at 336 and 621 nm, are attributed to n → Π{sup ⁎} transitions of electrons in C=O and S=O bonds, respectively. S,N-GQDs are highly luminescent and showed excitation dependent emission behaviors. Hybrid photosensing device has been fabricated with S,N-GQD sensitized ZnO nanorods and a conjugated polymer poly(3-hexylthiophene) (P3HT). S,N-GQD decorated ZnO nanorod demonstrated higher photoresponse compared to pristine ZnO nanorod based device. S,N-GQD/ZnO nanorod hybrid device showed superior incident photon to electron conversion efficiency (IPCE), photoresponsivity and detectivity compared to the control samples. The flexibility study of the samples has been monitored by measuring current-voltage characteristics at different bending angles. - Highlights: • S and N co-doped graphene quantum dots (S,N-GQDs) were synthesized. • ZnO nanorods were grown on ITO coated flexible PET substrates. • S,N-GQDs were attached with ZnO nanorods and used as a green sensitizer. • Photosensing properties of S,N-GQD/ZnO and P3HT polymer hybrid device was studied.
Quantum chemistry on a superconducting quantum processor
Energy Technology Data Exchange (ETDEWEB)
Kaicher, Michael P.; Wilhelm, Frank K. [Theoretical Physics, Saarland University, 66123 Saarbruecken (Germany); Love, Peter J. [Department of Physics and Astronomy, Tufts University, Medford, MA 02155 (United States)
2016-07-01
Quantum chemistry is the most promising civilian application for quantum processors to date. We study its adaptation to superconducting (sc) quantum systems, computing the ground state energy of LiH through a variational hybrid quantum classical algorithm. We demonstrate how interactions native to sc qubits further reduce the amount of quantum resources needed, pushing sc architectures as a near-term candidate for simulations of more complex atoms/molecules.
Lv, Ouyang; Tao, Yongxin; Qin, Yong; Chen, Chuanxiang; Pan, Yan; Deng, Linhong; Liu, Li; Kong, Yong
2016-10-01
Highly fluorescent graphene quantum dots (GQDs)-chitosan (CS) hybrid xerogels (GQDs-CS) were facilely synthesized, and the morphology of GQDs-CS was controllable by varying the content of GQDs in the xerogel. The GQDs-CS exhibited a porous and three-dimensional (3D) network structure when the content of GQDs reached 43% (wt%) in the xerogel, which was beneficial for drug loading and sustained release. The as-prepared GQDs-CS could also be applied for in vivo imaging since it showed strong blue, green and red luminescence under excitation of varying wavelengths. Moreover, the pH-induced protonation/deprotonation of the -NH2 groups on CS chains can result in a pH-dependent drug delivery behavior of the GQDs-CS hybrid xerogel. Copyright © 2016 Elsevier B.V. All rights reserved.
Noor, M Omair; Tavares, Anthony J; Krull, Ulrich J
2013-07-25
A microfluidic based solid-phase assay for the multiplexed detection of nucleic acid hybridization using quantum dot (QD) mediated fluorescence resonance energy transfer (FRET) is described herein. The glass surface of hybrid glass-polydimethylsiloxane (PDMS) microfluidic channels was chemically modified to assemble the biorecognition interface. Multiplexing was demonstrated using a detection system that was comprised of two colors of immobilized semi-conductor QDs and two different oligonucleotide probe sequences. Green-emitting and red-emitting QDs were paired with Cy3 and Alexa Fluor 647 (A647) labeled oligonucleotides, respectively. The QDs served as energy donors for the transduction of dye labeled oligonucleotide targets. The in-channel assembly of the biorecognition interface and the subsequent introduction of oligonucleotide targets was accomplished within minutes using a combination of electroosmotic flow and electrophoretic force. The concurrent quantification of femtomole quantities of two target sequences was possible by measuring the spatial coverage of FRET sensitized emission along the length of the channel. In previous reports, multiplexed QD-FRET hybridization assays that employed a ratiometric method for quantification had challenges associated with lower analytical sensitivity arising from both donor and acceptor dilution that resulted in reduced energy transfer pathways as compared to single-color hybridization assays. Herein, a spatial method for quantification that is based on in-channel QD-FRET profiles provided higher analytical sensitivity in the multiplexed assay format as compared to single-color hybridization assays. The selectivity of the multiplexed hybridization assays was demonstrated by discrimination between a fully-complementary sequence and a 3 base pair sequence at a contrast ratio of 8 to 1. Copyright © 2013 Elsevier B.V. All rights reserved.
Energy Technology Data Exchange (ETDEWEB)
Bazin, Alexandre; Monnier, Paul; Beaudoin, Grégoire; Sagnes, Isabelle; Raj, Rama [Laboratoire de Photonique et de Nanostructures (CNRS UPR20), Route de Nozay, Marcoussis 91460 (France); Lenglé, Kevin; Gay, Mathilde; Bramerie, Laurent [Université Européenne de Bretagne (UEB), 5 Boulevard Laënnec, 35000 Rennes (France); CNRS-Foton Laboratory (UMR 6082), Enssat, BP 80518, 22305 Lannion Cedex (France); Braive, Rémy; Raineri, Fabrice, E-mail: fabrice.raineri@lpn.cnrs.fr [Laboratoire de Photonique et de Nanostructures (CNRS UPR20), Route de Nozay, Marcoussis 91460 (France); Université Paris Diderot, Sorbonne Paris Cité, 75207 Paris Cedex 13 (France)
2014-01-06
Ultrafast switching with low energies is demonstrated using InP photonic crystal nanocavities embedding InGaAs surface quantum wells heterogeneously integrated to a silicon on insulator waveguide circuitry. Thanks to the engineered enhancement of surface non radiative recombination of carriers, switching time is obtained to be as fast as 10 ps. These hybrid nanostructures are shown to be capable of achieving systems level performance by demonstrating error free wavelength conversion at 10 Gbit/s with 6 mW switching powers.
Ema, K.; Inomata, M.; Kato, Y.; Kunugita, H.; Era, M.
2008-06-01
We report the observation of extremely efficient energy transfer (greater than 99%) in an organic-inorganic hybrid quantum-well structure consisting of perovskite-type lead bromide well layers and naphthalene-linked ammonium barrier layers. Time-resolved photoluminescence measurements confirm that the transfer is triplet-triplet Dexter-type energy transfer from Wannier excitons in the inorganic well to the triplet state of naphthalene molecules in the organic barrier. Using measurements in the 10 300 K temperature range, we also investigated the temperature dependence of the energy transfer.
Algar, W Russ; Krull, Ulrich J
2011-01-01
The use of quantum dots (QDs) as donors in fluorescence resonance energy transfer (FRET) offer several advantages for the development of multiplexed solid-phase QD-FRET nucleic acid hybridization assays. Designs for multiplexing have been demonstrated, but important challenges remain in the optimization of these systems. In this work, we identify several strategies based on the design of interfacial chemistry for improving sensitivity, obtaining lower limits of detection (LOD) and enabling the regeneration and reuse of solid-phase QD-FRET hybridization assays. FRET-sensitized emission from acceptor dyes associated with hybridization events at immobilized QD donors provides the analytical signal in these assays. The minimization of active sensing area reduces background from QD donor PL and allows the resolution of smaller amounts of acceptor emission, thus lowering the LOD. The association of multiple acceptor dyes with each hybridization event can enhance FRET efficiency, thereby improving sensitivity. Many previous studies have used interfacial protein layers to generate selectivity; however, transient destabilization of these layers is shown to prevent efficient regeneration. To this end, we report a protein-free interfacial chemistry and demonstrate the specific detection of as little as 2 pmol of target, as well as an improved capacity for regeneration.
Rudno-Rudziński, W.; Biegańska, D.; Misiewicz, J.; Lelarge, F.; Rousseau, B.; Sek, G.
2018-01-01
We investigate the diffusion of photo-generated carriers (excitons) in hybrid two dimensional-zero dimensional tunnel injection structures, based on strongly elongated InAs quantum dots (called quantum dashes, QDashes) of various heights, designed for emission at around 1.5 μm, separated by a 3.5 nm wide barrier from an 8 nm wide In0.64Ga0.36As0.78P0.22 quantum well (QW). By measuring the spectrally filtered real space images of the photoluminescence patterns with high resolution, we probe the spatial extent of the emission from QDashes. Deconvolution with the exciting light spot shape allows us to extract the carrier/exciton diffusion lengths. For the non-resonant excitation case, the diffusion length depends strongly on excitation power, pointing at carrier interactions and phonons as its main driving mechanisms. For the case of excitation resonant with absorption in the adjacent QW, the diffusion length does not depend on excitation power for low excitation levels since the generated carriers do not have sufficient excess kinetic energy. It is also found that the diffusion length depends on the quantum-mechanical coupling strength between QW and QDashes, controlled by changing the dash size. It influences the energy difference between the QDash ground state of the system and the quantum well levels, which affects the tunneling rates. When that QW-QDash level separation decreases, the probability of capturing excitons generated in the QW by QDashes increases, which is reflected by the decreased diffusion length from approx. 5 down to 3 μm.
Tahvili, M S; Du, L; Heck, M J R; Nötzel, R; Smit, M K; Bente, E A J M
2012-03-26
We present an investigation of passive and hybrid mode-locking in Fabry-Pérot type two-section InAs/InP(100) quantum dot lasers that show dual wavelength operation. Over the whole current and voltage range for mode-locking of these lasers, the optical output spectra show two distinct lobes. The two lobes provide a coherent bandwidth and are verified to lead to two synchronized optical pulses. The generated optical pulses are elongated in time due to a chirp which shows opposite signs over the two spectral lobes. Self-induced mode-locking in the single-section laser shows that the dual-wavelength spectra correspond to emission from ground state. In the hybrid mode-locking regime, a map of locking range is presented by measuring the values of timing jitter for several values of power and frequency of the external electrical modulating signal. An overview of the systematic behavior of InAs/InP(100) quantum dot mode-locked lasers is presented as conclusion.
Liu, Xiaoying; McBride, Sean P.; Jaeger, Heinrich M.; Nealey, Paul F.
2016-07-01
Hybrid nanomaterials comprised of well-organized arrays of colloidal semiconductor quantum dots (QDs) in close proximity to metal nanoparticles (NPs) represent an appealing system for high-performance, spectrum-tunable photon sources with controlled photoluminescence. Experimental realization of such materials requires well-defined QD arrays and precisely controlled QD-metal interspacing. This long-standing challenge is tackled through a strategy that synergistically combines lateral confinement and vertical stacking. Lithographically generated nanoscale patterns with tailored surface chemistry confine the QDs into well-organized arrays with high selectivity through chemical pattern directed assembly, while subsequent coating with a monolayer of close-packed Au NPs introduces the plasmonic component for fluorescence enhancement. The results show uniform fluorescence emission in large-area ordered arrays for the fabricated QD structures and demonstrate five-fold fluorescence amplification for red, yellow, and green QDs in the presence of the Au NP monolayer. Encapsulation of QDs with a silica shell is shown to extend the design space for reliable QD/metal coupling with stronger enhancement of 11 times through the tuning of QD-metal spatial separation. This approach provides new opportunities for designing hybrid nanomaterials with tailored array structures and multiple functionalities for applications such as multiplexed optical coding, color display, and quantum transduction.
Akimov, I. A.; Salewski, M.; Kalitukha, I. V.; Poltavtsev, S. V.; Debus, J.; Kudlacik, D.; Sapega, V. F.; Kopteva, N. E.; Kirstein, E.; Zhukov, E. A.; Yakovlev, D. R.; Karczewski, G.; Wiater, M.; Wojtowicz, T.; Korenev, V. L.; Kusrayev, Yu. G.; Bayer, M.
2017-11-01
The exchange interaction between magnetic ions and charge carriers in semiconductors is considered to be a prime tool for spin control. Here, we solve a long-standing problem by uniquely determining the magnitude of the long-range p -d exchange interaction in a ferromagnet-semiconductor (FM-SC) hybrid structure where a 10-nm-thick CdTe quantum well is separated from the FM Co layer by a CdMgTe barrier with a thickness on the order of 10 nm. The exchange interaction is manifested by the spin splitting of acceptor bound holes in the effective magnetic field induced by the FM. The exchange splitting is directly evaluated using spin-flip Raman scattering by analyzing the dependence of the Stokes shift ΔS on the external magnetic field B . We show that in a strong magnetic field, ΔS is a linear function of B with an offset of Δp d=50 -100 μ eV at zero field from the FM induced effective exchange field. On the other hand, the s -d exchange interaction between conduction band electrons and FM, as well as the p -d contribution for free valence band holes, are negligible. The results are well described by the model of indirect exchange interaction between acceptor bound holes in the CdTe quantum well and the FM layer mediated by elliptically polarized phonons in the hybrid structure.
Chen, Lu; Algar, W Russ; Tavares, Anthony J; Krull, Ulrich J
2011-01-01
The optical properties and surface area of quantum dots (QDs) have made them an attractive platform for the development of nucleic acid biosensors based on fluorescence resonance energy transfer (FRET). Solid-phase assays based on FRET using mixtures of immobilized QD-oligonucleotide conjugates (QD biosensors) have been developed. The typical challenges associated with solid-phase detection strategies include non-specific adsorption, slow kinetics of hybridization, and sample manipulation. The new work herein has considered the immobilization of QD biosensors onto the surfaces of microfluidic channels in order to address these challenges. Microfluidic flow can be used to dynamically control stringency by adjustment of the potential in an electrokinetic-based microfluidics environment. The shearing force, Joule heating, and the competition between electroosmotic and electrophoretic mobilities allow the optimization of hybridization conditions, convective delivery of target to the channel surface to speed hybridization, amelioration of adsorption, and regeneration of the sensing surface. Microfluidic flow can also be used to deliver (for immobilization) and remove QD biosensors. QDs that were conjugated with two different oligonucleotide sequences were used to demonstrate feasibility. One oligonucleotide sequence on the QD was available as a linker for immobilization via hybridization with complementary oligonucleotides located on a glass surface within a microfluidic channel. A second oligonucleotide sequence on the QD served as a probe to transduce hybridization with target nucleic acid in a sample solution. A Cy3 label on the target was excited by FRET using green-emitting CdSe/ZnS QD donors and provided an analytical signal to explore this detection strategy. The immobilized QDs could be removed under denaturing conditions by disrupting the duplex that was used as the surface linker and thus allowed a new layer of QD biosensors to be re-coated within the channel
Noor, M Omair; Krull, Ulrich J
2013-08-06
A multiplexed solid-phase nucleic acid hybridization assay on a paper-based platform is presented using multicolor immobilized quantum dots (QDs) as donors in fluorescence resonance energy transfer (FRET). The surface of paper was modified with imidazole groups to immobilize two types of QD-probe oligonucleotide conjugates that were assembled in solution. Green-emitting QDs (gQDs) and red-emitting QDs (rQDs) served as donors with Cy3 and Alexa Fluor 647 (A647) acceptors. The gQD/Cy3 FRET pair served as an internal standard, while the rQD/A647 FRET pair served as a detection channel, combining the control and analytical test zones in one physical location. Hybridization of dye-labeled oligonucleotide targets provided the proximity for FRET sensitized emission from the acceptor dyes, which served as an analytical signal. Hybridization assays in the multicolor format provided a limit of detection of 90 fmol and an upper limit of dynamic range of 3.5 pmol. The use of an array of detection zones was designed to provide improved analytical figures of merit compared to that which could be achieved on one type of array design in terms of relative concentration of multicolor QDs. The hybridization assays showed excellent resistance to nonspecific adsorption of oligonucleotides. Selectivity of the two-plex hybridization assay was demonstrated by single nucleotide polymorphism (SNP) detection at a contrast ratio of 50:1. Additionally, it is shown that the use of preformed QD-probe oligonucleotide conjugates and consideration of the relative number density of the two types of QD-probe conjugates in the two-color assay format is advantageous to maximize assay sensitivity and the upper limit of dynamic range.
Quantum Security of Cryptographic Primitives
Gagliardoni, Tommaso
2017-01-01
We call quantum security the area of IT security dealing with scenarios where one or more parties have access to quantum hardware. This encompasses both the fields of post-quantum cryptography (that is, traditional cryptography engineered to be resistant against quantum adversaries), and quantum cryptography (that is, security protocols designed to be natively run on a quantum infrastructure, such as quantum key distribution). Moreover, there exist also hybrid models, where traditional crypto...
Hatef, Ali; Sadeghi, Seyed M; Fortin-Deschênes, Simon; Boulais, Etienne; Meunier, Michel
2013-03-11
It is well-known that optical properties of semiconductor quantum dots can be controlled using optical cavities or near fields of localized surface plasmon resonances (LSPRs) of metallic nanoparticles. In this paper we study the optics, energy transfer pathways, and exciton states of quantum dots when they are influenced by the near fields associated with plasmonic meta-resonances. Such resonances are formed via coherent coupling of excitons and LSPRs when the quantum dots are close to metallic nanorods and driven by a laser beam. Our results suggest an unprecedented sensitivity to the refractive index of the environment, causing significant spectral changes in the Förster resonance energy transfer from the quantum dots to the nanorods and in exciton transition energies. We demonstrate that when a quantum dot-metallic nanorod system is close to its plasmonic meta-resonance, we can adjust the refractive index to: (i) control the frequency range where the energy transfer from the quantum dot to the metallic nanorod is inhibited, (ii) manipulate the exciton transition energy shift of the quantum dot, and (iii) disengage the quantum dot from the metallic nanoparticle and laser field. Our results show that near meta-resonances the spectral forms of energy transfer and exciton energy shifts are strongly correlated to each other.
Gao, Jiali; Major, Dan T; Fan, Yao; Lin, Yen-Lin; Ma, Shuhua; Wong, Kin-Yiu
2008-01-01
A method for incorporating quantum mechanics into enzyme kinetics modeling is presented. Three aspects are emphasized: 1) combined quantum mechanical and molecular mechanical methods are used to represent the potential energy surface for modeling bond forming and breaking processes, 2) instantaneous normal mode analyses are used to incorporate quantum vibrational free energies to the classical potential of mean force, and 3) multidimensional tunneling methods are used to estimate quantum effects on the reaction coordinate motion. Centroid path integral simulations are described to make quantum corrections to the classical potential of mean force. In this method, the nuclear quantum vibrational and tunneling contributions are not separable. An integrated centroid path integral-free energy perturbation and umbrella sampling (PI-FEP/UM) method along with a bisection sampling procedure was summarized, which provides an accurate, easily convergent method for computing kinetic isotope effects for chemical reactions in solution and in enzymes. In the ensemble-averaged variational transition state theory with multidimensional tunneling (EA-VTST/MT), these three aspects of quantum mechanical effects can be individually treated, providing useful insights into the mechanism of enzymatic reactions. These methods are illustrated by applications to a model process in the gas phase, the decarboxylation reaction of N-methyl picolinate in water, and the proton abstraction and reprotonation process catalyzed by alanine racemase. These examples show that the incorporation of quantum mechanical effects is essential for enzyme kinetics simulations.
Directory of Open Access Journals (Sweden)
Abdullah M. Iliyasu
2017-12-01
Full Text Available A quantum hybrid (QH intelligent approach that blends the adaptive search capability of the quantum-behaved particle swarm optimisation (QPSO method with the intuitionistic rationality of traditional fuzzy k-nearest neighbours (Fuzzy k-NN algorithm (known simply as the Q-Fuzzy approach is proposed for efficient feature selection and classification of cells in cervical smeared (CS images. From an initial multitude of 17 features describing the geometry, colour, and texture of the CS images, the QPSO stage of our proposed technique is used to select the best subset features (i.e., global best particles that represent a pruned down collection of seven features. Using a dataset of almost 1000 images, performance evaluation of our proposed Q-Fuzzy approach assesses the impact of our feature selection on classification accuracy by way of three experimental scenarios that are compared alongside two other approaches: the All-features (i.e., classification without prior feature selection and another hybrid technique combining the standard PSO algorithm with the Fuzzy k-NN technique (P-Fuzzy approach. In the first and second scenarios, we further divided the assessment criteria in terms of classification accuracy based on the choice of best features and those in terms of the different categories of the cervical cells. In the third scenario, we introduced new QH hybrid techniques, i.e., QPSO combined with other supervised learning methods, and compared the classification accuracy alongside our proposed Q-Fuzzy approach. Furthermore, we employed statistical approaches to establish qualitative agreement with regards to the feature selection in the experimental scenarios 1 and 3. The synergy between the QPSO and Fuzzy k-NN in the proposed Q-Fuzzy approach improves classification accuracy as manifest in the reduction in number cell features, which is crucial for effective cervical cancer detection and diagnosis.
Kim, Taesoo; Firdaus, Yuliar; Kirmani, Ahmad R.; Liang, Ru-Ze; Hu, Hanlin; Liu, Mengxia; El Labban, Abdulrahman; Hoogland, Sjoerd; Beaujuge, Pierre; Sargent, Edward H.; Amassian, Aram
2018-01-01
Realization of colloidal quantum dot (CQD)/organic photovoltaic (OPV) tandem solar cells that integrate the strong infrared absorption of CQDs with large photovoltages of OPVs is an attractive option toward high-performing, low-cost thin film solar
International Nuclear Information System (INIS)
Ruiyi, Li; Yuanyuan, Jiang; Xiaoyan, Zhou; Zaijun, Li; Zhiguo, Gu; Guangli, Wang; Junkang, Liu
2015-01-01
Graphical abstract: The study reported a facile synthesis of Li4Ti5O12/nitrogen and sulfur co-doped graphene quantum dots (LTO/N,S-GQDs). The unique architecture and the introduction of N,S-GQDs create both ultrafast electron transfer and electrolyte transport. The as-prepared LTO/N,S-GQDs anode provides prominent advantage of specific capacity, high-rate performance and cycle stability. - Highlights: • We reported a new lithium titanate/nitrogen and sulfur co-doped graphene quantum dots hybrid • The synthesis creates a crystalline interconnected porous framework composed of nanoscale LTO • The unique architecture achieves to maximize the rate performance and enhance the power density • Introduction of N,S-GQDs greatly enhances the electron transfer and the storage lithium capacity • The hybrid anode provides an excellent electrochemical performance for lithium-ion batteries - ABSTRACT: The paper reported a facile synthesis of lithium titanate/nitrogen and sulfur co-doped graphene quantum dots(LTO/N,S-GQDs). Tetrabutyl titanate was dissolved in tertbutanol and heated to refluxing state by microwave irradiation. Then, lithium acetate was added into the mixed solution to produce LTO precursor. The precursor was hybridized with N,S-GQDs in ethanol. Followed by drying and thermal annealing at 500 °C in Ar/H_2 to obtain LTO/N,S-GQDs. The synthesis creates fully crystalline interconnected porous framework composed of nanoscale LTO crystals. The unique architecture achieves to maximize the high-rate performance and enhance the power density. More importantly, the introduction of N,S-GQDs don't almost influence on the electrolyte transport, but greatly improve the electron transfer and the storage lithium capacity. The LTO/N,S-GQDs anode exhibits remarkably enhanced electrochemical performance for lithium ion battery. The specific discharge capacity is 254.2 mAh g"−"1 at 0.1C and 126.5 mAh g"−"1 at 10C. The capacity remains 96.9% at least after 2000 cycles
Amjadi, Mohammad; Jalili, Roghayeh
2018-02-01
We report on a ratiometric fluorescent sensor based on dual-emission molecularly imprinted mesoporous silica embedded with carbon dots and CdTe quantum dots (mMIP@CDs/QDs) for celecoxib (CLX) as target molecule. The fluorescence of the embedded CDs is insensitive to the analyte while the green emissive QDs are selectively quenched by it. This effect is much stronger for the MIP than for the non-imprinted polymer, which indicates a good recognition ability of the mesoporous MIP. The hybrid sensor also exhibited good selectivity to CLX over other substances. The ratio of the intensity at two wavelengths (F550/F440) proportionally decreased with the increasing of CLX concentration in the range of 0.08-0.90 μM. A detection limit as low as 57 nM was achieved. Experimental results testified that this sensor was highly sensitive and selective for the detection of CLX in human serum samples.
International Nuclear Information System (INIS)
Sadeghi, S M
2009-01-01
We study the inhibition of optical excitation and enhancement of Rabi flopping and frequency in semiconductor quantum dots via plasmonic effects. This is done by demonstrating that the interaction of a quantum dot with a laser field in the vicinity of a metallic nanoparticle can be described in terms of optical Bloch equations with a plasmically normalized Rabi frequency. We show that in the weak-field regime plasmonic effects can suppress the interband transitions, inhibiting exciton generation. In the strong-field regime these effects delay the response of the quantum dot to the laser field and enhance Rabi flopping. We relate these to the conversion of Rabi frequency from a real quantity into a complex and strongly frequency-dependent quantity as plasmonic effects become significant. We show that, within the strong-field regime, in the wavelength range where real and imaginary parts of this frequency reach their maxima, a strongly frequency-dependent enhancement of carrier excitation can happen.
DEFF Research Database (Denmark)
Curutchet, Carles; Cupellini, Lorenzo; Kongsted, Jacob
2018-01-01
embedding approaches, respectively, nonelectrostatic dispersion and repulsion interactions are instead commonly described through classical potentials despite their quantum mechanical origin. Here we present an extension of the Tkatchenko-Scheffler semiempirical van der Waals (vdWTS) scheme aimed......Mixed multiscale quantum/molecular mechanics (QM/MM) models are widely used to explore the structure, reactivity, and electronic properties of complex chemical systems. Whereas such models typically include electrostatics and potentially polarization in so-called electrostatic and polarizable...... at describing dispersion and repulsion interactions between quantum and classical regions within a QM/MM polarizable embedding framework. Starting from the vdWTSexpression, we define a dispersion and a repulsion term, both of them density-dependent and consistently based on a Lennard-Jones-like potential. We...
Boggio-Pasqua, Martial; Burmeister, Carl F; Robb, Michael A; Groenhof, Gerrit
2012-06-14
Organisms have evolved a wide variety of mechanisms to utilize and respond to light. In many cases, the biological response is mediated by structural changes that follow photon absorption in a protein complex. The initial step in such cases is normally the photoisomerization of a highly conjugated prosthetic group. To understand better the factors controlling the isomerization, we perform atomistic molecular dynamics simulations. In this perspective article we briefly review the key theoretical concepts of photochemical reactions and present a practical simulation scheme for simulating photochemical reactions in biomolecular systems. In our scheme, a multi-configurational quantum mechanical description is used to model the electronic rearrangement for those parts of the system that are involved in the photon absorption. For the remainder, typically consisting of the apo-protein and the solvent, a simple force field model is used. The interactions in the systems are thus computed within a hybrid quantum/classical framework. Forces are calculated on-the-fly, and a diabatic surface hopping procedure is used to model the excited-state decay. To demonstrate how this method is used we review our studies on photoactivation of the photoactive yellow protein, a bacterial photoreceptor. We will show what information can be obtained from the simulations, and, by comparing to recent experimental findings, what the limitations of our simulations are.
Jung, Hyunchul; Chung, Wonkeun; Lee, Chang Hun; Kim, Sung Hyun
2012-07-01
White light-emitting diodes (LEDs) were fabricated using GaN-based 380-nm UV LEDs precoated with the composite of blue-emitting polymer (poly[(9,9-dihexylfluorenyl-2,7-diyl)-alt-co-(2-methoxy-5-{2-ethylhexyloxy)-1 ,4-phenylene)]), yellow green-emitting polymer (poly[(9,9-dioctylfluorenyl-2,7-diyl)-co-(1,4-benzo-{2,1',3}-thiadiazole)]), and 605-nm red-emitting quantum dots (QDs). CdSe cores were obtained by solvothermal route using CdO, Se precursors and ZnS shells were synthesized by using diethylzinc, and hexamethyldisilathiane precursors. The optical properties of CdSe/ZnS QDs were characterized by UV-visible and photoluminescence (PL) spectra. The structural data and composition of the QDs were transmission electron microscopy (TEM), and EDX technique. The quantum yield and size of the QDs were 58.7% and about 6.7 nm, respectively. Three-band white light was generated by hybridizing blue (430 nm), green (535 nm), and red (605 nm) emission. The color-rendering index (CRI) of the device was extremely improved by introducing the QDs. The CIE-1931 chromaticity coordinate, color temperature, and CRI of a white LED at 20 mA were (0.379, 0.368), 3969 K, and 90, respectively.
Sanchez, Rafael S; de la Fuente, Mauricio Solis; Suarez, Isaac; Muñoz-Matutano, Guillermo; Martinez-Pastor, Juan P; Mora-Sero, Ivan
2016-01-01
We report the first observation of exciplex state electroluminescence due to carrier injection between the hybrid lead halide perovskite (MAPbI3-xClx) and quantum dots (core/shell PbS/CdS). Single layers of perovskite (PS) and quantum dots (QDs) have been produced by solution processing methods, and their photoluminescent properties are compared to those of bilayer samples in both PS/QD and QD/PS configurations. Exciplex emission at lower energies than the band gap of both PS and QD has been detected. The exciplex emission wavelength of this mixed system can be simply tuned by controlling the QD size. Light-emitting diodes (LEDs) have been fabricated using those configurations, which provide light emission with considerably low turn-on potential. The "color" of the LED can also be tuned by controlling the applied bias. The presence of the exciplex state PS and QDs opens up a broad range of possibilities with important implications not only in tunable LEDs but also in the preparation of intermediate band gap photovoltaic devices with the potentiality of surpassing the Shockley-Queisser limit.
Sanchez, Rafael S.; de la Fuente, Mauricio Solis; Suarez, Isaac; Muñoz-Matutano, Guillermo; Martinez-Pastor, Juan P.; Mora-Sero, Ivan
2016-01-01
We report the first observation of exciplex state electroluminescence due to carrier injection between the hybrid lead halide perovskite (MAPbI3–xClx) and quantum dots (core/shell PbS/CdS). Single layers of perovskite (PS) and quantum dots (QDs) have been produced by solution processing methods, and their photoluminescent properties are compared to those of bilayer samples in both PS/QD and QD/PS configurations. Exciplex emission at lower energies than the band gap of both PS and QD has been detected. The exciplex emission wavelength of this mixed system can be simply tuned by controlling the QD size. Light-emitting diodes (LEDs) have been fabricated using those configurations, which provide light emission with considerably low turn-on potential. The “color” of the LED can also be tuned by controlling the applied bias. The presence of the exciplex state PS and QDs opens up a broad range of possibilities with important implications not only in tunable LEDs but also in the preparation of intermediate band gap photovoltaic devices with the potentiality of surpassing the Shockley-Queisser limit. PMID:26844299
Chen, Miaoxiang; Kobashi, Kazufumi
2012-09-01
Hybridizing air-stable organic-molecules with advanced III-V semiconductor quantum-dots (QDs) structures can be utilized to create a new generation of biochemical sensing devices. In order to enhance their optical performances, the active regions in these QDs structures commonly consist of multistacked dots-in-a-well (DWELL) units. The effects of grafted molecules on the performances of the QDs structures with multistacked DWELLs, however, still remain unclear. Here, we show the significant improvements in the optical properties of InAs QDs in a hybrid nanosystem obtained by grafting biocompatible diazonium salt compound (amine donor) atop InAs QDs structure. Since its interface between the QDs structure and molecular monolayer retains an uncontaminated and non-oxidized condition, the nanosystem is an ideal platform to study the intrinsic properties of charge-carrier transport inside the system. Because of the complexity of the energy-levels in the QDs structure due to the existing surface QDs and DWELLs, selective excitation wavelengths (400, 633, and 885 nm, respectively) with different photo-energies are used to exactly analyze the complete charging mechanism in these QDs. A clear view of charge-carrier transfer inside the nanosystem is revealed by employing photoluminescence technique under selective-wavelength excitations. The present work provides new quantitative evidences for exploiting inorganic QDs applications in complex biological systems.
Energy Technology Data Exchange (ETDEWEB)
Chen Miaoxiang [Department of Micro- and Nano technology, Technical University of Denmark, Orsteds Plads, 2800 Kgs. Lyngby (Denmark); Kobashi, Kazufumi [Nanotube Research Center, National Institute of Advanced Industrial Science and Technology (AIST), AIST Tsukuba Central 5, 1-1-1 Higashi, Tsukuba, Ibaraki 305-8565 (Japan)
2012-09-15
Hybridizing air-stable organic-molecules with advanced III-V semiconductor quantum-dots (QDs) structures can be utilized to create a new generation of biochemical sensing devices. In order to enhance their optical performances, the active regions in these QDs structures commonly consist of multistacked dots-in-a-well (DWELL) units. The effects of grafted molecules on the performances of the QDs structures with multistacked DWELLs, however, still remain unclear. Here, we show the significant improvements in the optical properties of InAs QDs in a hybrid nanosystem obtained by grafting biocompatible diazonium salt compound (amine donor) atop InAs QDs structure. Since its interface between the QDs structure and molecular monolayer retains an uncontaminated and non-oxidized condition, the nanosystem is an ideal platform to study the intrinsic properties of charge-carrier transport inside the system. Because of the complexity of the energy-levels in the QDs structure due to the existing surface QDs and DWELLs, selective excitation wavelengths (400, 633, and 885 nm, respectively) with different photo-energies are used to exactly analyze the complete charging mechanism in these QDs. A clear view of charge-carrier transfer inside the nanosystem is revealed by employing photoluminescence technique under selective-wavelength excitations. The present work provides new quantitative evidences for exploiting inorganic QDs applications in complex biological systems.
International Nuclear Information System (INIS)
Islam, S. M. Z.; Gayen, Taposh; Tint, Naing; Alfano, Robert; Shi, Lingyan; Seredych, Mykola; Bandosz, Teresa J.
2014-01-01
The effects of fabrication temperature are investigated on the performance of CdSe quantum dot (QD)-sensitized hybrid solar cells of the composite material of zinc (hydr)oxide (ZnOH-GO)with 2 wt. % graphite oxide. The current-voltage (I-V) and photo-current measurements show that higher fabrication temperatures yield greater photovoltaic power conversion efficiencies that essentially indicate more efficient solar cells. Two Photon Fluorescence images show the effects of temperature on the internal morphologies of the solar devices based on such materials. The CdSe-QD sensitized ZnOH-GO hybrid solar cells fabricated at 450 °C showing conversion of ∼10.60% under a tungsten lamp (12.1 mW/cm 2 ) are reported here, while using potassium iodide as an electrolyte. The output photocurrent, I (μA) with input power, P (mW/cm 2 ) is found to be superlinear, showing a relation of I = P n , where n = 1.4.
Youn, Duck Hyun; Seol, Minsu; Kim, Jae Young; Jang, Ji-Wook; Choi, Youngwoo; Yong, Kijung; Lee, Jae Sung
2013-02-01
The development of an efficient noble-metal-free counter electrode is crucial for possible applications of quantum-dot-sensitized solar cells (QDSSCs). Herein, we present TiN nanoparticles on a carbon nanotube (CNT)-graphene hybrid support as a noble-metal-free counter electrode for QDSSCs employing a polysulfide electrolyte. The resulting TiN/CNT-graphene possesses an extremely high surface roughness, a good metal-support interaction, and less aggregation relative to unsupported TiN; it also has superior solar power conversion efficiency (4.13 %) when applying a metal mask, which is much higher than that of the state-of-the-art Au electrode (3.35 %). Based on electrochemical impedance spectroscopy measurements, the enhancement is ascribed to a synergistic effect between TiN nanoparticles and the CNT-graphene hybrid, the roles of which are to provide active sites for the reduction of polysulfide ions and electron pathways to TiN nanoparticles, respectively. The combination of graphene and CNTs leads to a favorable morphology that prevents stacking of graphene or bundling of CNTs, which maximizes the contact of the support with TiN nanoparticles and improves electron-transfer capability relative to either carbon material alone. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Doughan, Samer; Uddayasankar, Uvaraj; Krull, Ulrich J
2015-06-09
Monodisperse aqueous upconverting nanoparticles (UCNPs) were covalently immobilized on aldehyde modified cellulose paper via reduction amination to develop a luminescence resonance energy transfer (LRET)-based nucleic acid hybridization assay. This first account of covalent immobilization of UCNPs on paper for a bioassay reports an optically responsive method that is sensitive, reproducible and robust. The immobilized UCNPs were decorated with oligonucleotide probes to capture HPRT1 housekeeping gene fragments, which in turn brought reporter conjugated quantum dots (QDs) in close proximity to the UCNPs for LRET. This sandwich assay could detect unlabeled oligonucleotide target, and had a limit of detection of 13 fmol and a dynamic range spanning nearly 3 orders of magnitude. The use of QDs, which are excellent LRET acceptors, demonstrated improved sensitivity, limit of detection, dynamic range and selectivity compared to similar assays that have used molecular fluorophores as acceptors. The selectivity of the assay was attributed to the decoration of the QDs with polyethylene glycol to eliminate non-specific adsorption. The kinetics of hybridization were determined to be diffusion limited and full signal development occurred within 3 min. Copyright © 2015 Elsevier B.V. All rights reserved.
International Nuclear Information System (INIS)
Kim, Kyungnam; Jeong, Sohee; Woo, Ju Yeon; Han, Chang-Soo
2012-01-01
We report successive and large-scale synthesis of InP/ZnS core/shell nanocrystal quantum dots (QDs) using a customized hybrid flow reactor, which is based on serial combination of a batch-type mixer and a flow-type furnace. InP cores and InP/ZnS core/shell QDs were successively synthesized in the hybrid reactor in a simple one-step process. In this reactor, the flow rate of the solutions was typically 1 ml min −1 , 100 times larger than that of conventional microfluidic reactors. In order to synthesize high-quality InP/ZnS QDs, we controlled both the flow rate and the crystal growth temperature. Finally, we obtained high-quality InP/ZnS QDs in colors from bluish green to red, and we demonstrated that these core/shell QDs could be incorporated into white-light-emitting diode (LED) devices to improve color rendering performance. (paper)
Kim, Kyungnam; Jeong, Sohee; Woo, Ju Yeon; Han, Chang-Soo
2012-02-01
We report successive and large-scale synthesis of InP/ZnS core/shell nanocrystal quantum dots (QDs) using a customized hybrid flow reactor, which is based on serial combination of a batch-type mixer and a flow-type furnace. InP cores and InP/ZnS core/shell QDs were successively synthesized in the hybrid reactor in a simple one-step process. In this reactor, the flow rate of the solutions was typically 1 ml min-1, 100 times larger than that of conventional microfluidic reactors. In order to synthesize high-quality InP/ZnS QDs, we controlled both the flow rate and the crystal growth temperature. Finally, we obtained high-quality InP/ZnS QDs in colors from bluish green to red, and we demonstrated that these core/shell QDs could be incorporated into white-light-emitting diode (LED) devices to improve color rendering performance.
Moix, Jeremy M.; Cao, Jianshu
2013-10-01
The hierarchical equations of motion technique has found widespread success as a tool to generate the numerically exact dynamics of non-Markovian open quantum systems. However, its application to low temperature environments remains a serious challenge due to the need for a deep hierarchy that arises from the Matsubara expansion of the bath correlation function. Here we present a hybrid stochastic hierarchical equation of motion (sHEOM) approach that alleviates this bottleneck and leads to a numerical cost that is nearly independent of temperature. Additionally, the sHEOM method generally converges with fewer hierarchy tiers allowing for the treatment of larger systems. Benchmark calculations are presented on the dynamics of two level systems at both high and low temperatures to demonstrate the efficacy of the approach. Then the hybrid method is used to generate the exact dynamics of systems that are nearly impossible to treat by the standard hierarchy. First, exact energy transfer rates are calculated across a broad range of temperatures revealing the deviations from the Förster rates. This is followed by computations of the entanglement dynamics in a system of two qubits at low temperature spanning the weak to strong system-bath coupling regimes.
International Nuclear Information System (INIS)
Bizarro, J.P.
1993-10-01
A comprehensive and detailed investigation is presented on the dynamics of the lower hybrid wave during current drive in tokamaks in situations where toroidally induced ray stochasticity is important and on the Weyl-Wigner formalism for rotation angle and angular momentum variables in quantum mechanics. It is shown that ray-tracing and Fokker-Planck codes are reliable tools for modelling the physics of lower-hybrid current drive provided a large number of rays is used when stochastic effects are important, and, in particular, that such codes are capable of reproducing the experimentally observed features of the hard X-ray emission. The balance between the wave damping and the stochastic divergence of nearby ray trajectories appears to be of great importance in governing the dynamics of the launched power spectrum and in establishing the characteristics of the deposition patterns. The implications of rotational periodicity and of angular momentum quantization for the Weyl-Wigner formalism are analyzed. Particular attention is paid to discreteness and its consequences: importance of evenness and oddness, use of two difference operators instead of one differential operator. 24 refs
Ziaei, Vafa; Bredow, Thomas
2017-03-17
The reliable calculation of the excited states of charge-transfer (CT) compounds poses a major challenge to the ab initio community because the frequently employed method, time-dependent density functional theory (TD-DFT), massively relies on the underlying density functional, resulting in heavily Hartree-Fock (HF) exchange-dependent excited-state energies. By applying the highly sophisticated many-body perturbation approach, we address the encountered unreliabilities and inconsistencies of not optimally tuned (standard) TD-DFT regarding photo-excited CT phenomena, and present results concerning accurate vertical transition energies and the correct energetic ordering of the CT and the first visible singlet state of a recently synthesized thermodynamically stable large hybrid perylene bisimide-macrocycle complex. This is a large-scale application of the quantum many-body perturbation approach to a chemically relevant CT system, demonstrating the system-size independence of the quality of the many-body-based excitation energies. Furthermore, an optimal tuning of the ωB97X hybrid functional can well reproduce the many-body results, making TD-DFT a suitable choice but at the expense of introducing a range-separation parameter, which needs to be optimally tuned. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.
Yin, Yuhang; Luan, Weiling; Zhang, Chengxi; Yang, Fuqian
2017-12-01
Recently, all-inorganic perovskites CsPbX3 (X= Cl, Br and I) quantum dots (QDs) have drawn great attentions because of their PL spectra tunable over the whole visible spectral region (400-700 nm) and adjustable bandgap, which revealed a promising potential on the field of photoelectronic devices, such as solar cells, LEDs and sensors. In this paper, CsPbX3 QDs and hybrid QDs, CsPbClxBr3-x and CsPbBrxI3-x were synthesized via one-step and two-step methods comparably. The optical bandgaps of CsPbCl3, CsPbBr3, and CsPbI3, were calculated as 3.08, 2.36, and 1.73eV, respectively, based on the Tauc’s equation and UV absorption spectra. Ionic displacement and phase transformation occurred during the mixing process were found based on the monitoring of PL spectra and HRTEM characterization. The long-term stability, dried, high quality and two-dimensional hybrid CsPbBrxI3-x QDs powders could be achieved via the two-step method. Polar solution inductions were used to wash and purify the CsPbX3 QDs, which help obtain of various compositions and well crystallize all-inorganic perovskites QDs powders.
Energy Technology Data Exchange (ETDEWEB)
Firdaus, Yuliar; Van der Auweraer, Mark, E-mail: mark.vanderauweraer@chem.kuleuven.be [Laboratory of Photochemistry and Spectroscopy, Division of Molecular Imaging and Photonics, Chemistry Department, KULeuven, Celestijnenlaan 200F, 2404, B-3001 Leuven (Belgium); Vandenplas, Erwin; Gehlhaar, Robert; Cheyns, David [Imec vzw, Kapeldreef 75, B-3001 Leuven (Belgium); Justo, Yolanda; Hens, Zeger [Physical Chemistry Laboratory, Ghent University, Krijgslaan 281-S3, 9000 Gent (Belgium)
2014-09-07
Different approaches of surface modification of the quantum dots (QDs), namely, solution-phase (octylamine, octanethiol) and post-deposition (acetic acid, 1,4-benzenedithiol) ligand exchange were used in the fabrication of hybrid bulk heterojunction solar cell containing poly (3-hexylthiophene) (P3HT) and small (2.4 nm) PbS QDs. We show that replacing oleic acid by shorter chain ligands improves the figures of merit of the solar cells. This can possibly be attributed to a combination of a reduced thickness of the barrier for electron transfer and an optimized phase separation. The best results were obtained for post-deposition ligand exchange by 1,4-benzenedithiol, which improves the power conversion efficiency of solar cells based on a bulk heterojunction of lead sulfide (PbS) QDs and P3HT up to two orders of magnitude over previously reported hybrid cells based on a bulk heterojunction of P3HT:PbS QDs, where the QDs are capped by acetic acid ligands. The optimal performance was obtained for solar cells with 69 wt. % PbS QDs. Besides the ligand effects, the improvement was attributed to the formation of an energetically favorable bulk heterojunction with P3HT, when small size (2.4 nm) PbS QDs were used. Dark current density-voltage (J-V) measurements carried out on the device provided insight into the working mechanism: the comparison between the dark J-V characteristics of the bench mark system P3HT:PCBM and the P3HT:PbS blends allows us to conclude that a larger leakage current and a more efficient recombination are the major factors responsible for the larger losses in the hybrid system.
International Nuclear Information System (INIS)
Firdaus, Yuliar; Van der Auweraer, Mark; Vandenplas, Erwin; Gehlhaar, Robert; Cheyns, David; Justo, Yolanda; Hens, Zeger
2014-01-01
Different approaches of surface modification of the quantum dots (QDs), namely, solution-phase (octylamine, octanethiol) and post-deposition (acetic acid, 1,4-benzenedithiol) ligand exchange were used in the fabrication of hybrid bulk heterojunction solar cell containing poly (3-hexylthiophene) (P3HT) and small (2.4 nm) PbS QDs. We show that replacing oleic acid by shorter chain ligands improves the figures of merit of the solar cells. This can possibly be attributed to a combination of a reduced thickness of the barrier for electron transfer and an optimized phase separation. The best results were obtained for post-deposition ligand exchange by 1,4-benzenedithiol, which improves the power conversion efficiency of solar cells based on a bulk heterojunction of lead sulfide (PbS) QDs and P3HT up to two orders of magnitude over previously reported hybrid cells based on a bulk heterojunction of P3HT:PbS QDs, where the QDs are capped by acetic acid ligands. The optimal performance was obtained for solar cells with 69 wt. % PbS QDs. Besides the ligand effects, the improvement was attributed to the formation of an energetically favorable bulk heterojunction with P3HT, when small size (2.4 nm) PbS QDs were used. Dark current density-voltage (J-V) measurements carried out on the device provided insight into the working mechanism: the comparison between the dark J-V characteristics of the bench mark system P3HT:PCBM and the P3HT:PbS blends allows us to conclude that a larger leakage current and a more efficient recombination are the major factors responsible for the larger losses in the hybrid system
Curutchet, Carles; Cupellini, Lorenzo; Kongsted, Jacob; Corni, Stefano; Frediani, Luca; Steindal, Arnfinn Hykkerud; Guido, Ciro A; Scalmani, Giovanni; Mennucci, Benedetta
2018-03-13
Mixed multiscale quantum/molecular mechanics (QM/MM) models are widely used to explore the structure, reactivity, and electronic properties of complex chemical systems. Whereas such models typically include electrostatics and potentially polarization in so-called electrostatic and polarizable embedding approaches, respectively, nonelectrostatic dispersion and repulsion interactions are instead commonly described through classical potentials despite their quantum mechanical origin. Here we present an extension of the Tkatchenko-Scheffler semiempirical van der Waals (vdW TS ) scheme aimed at describing dispersion and repulsion interactions between quantum and classical regions within a QM/MM polarizable embedding framework. Starting from the vdW TS expression, we define a dispersion and a repulsion term, both of them density-dependent and consistently based on a Lennard-Jones-like potential. We explore transferable atom type-based parametrization strategies for the MM parameters, based on either vdW TS calculations performed on isolated fragments or on a direct estimation of the parameters from atomic polarizabilities taken from a polarizable force field. We investigate the performance of the implementation by computing self-consistent interaction energies for the S22 benchmark set, designed to represent typical noncovalent interactions in biological systems, in both equilibrium and out-of-equilibrium geometries. Overall, our results suggest that the present implementation is a promising strategy to include dispersion and repulsion in multiscale QM/MM models incorporating their explicit dependence on the electronic density.
Noor, M Omair; Krull, Ulrich J
2014-10-21
Paper-based diagnostic assays are gaining increasing popularity for their potential application in resource-limited settings and for point-of-care screening. Achievement of high sensitivity with precision and accuracy can be challenging when using paper substrates. Herein, we implement the red-green-blue color palette of a digital camera for quantitative ratiometric transduction of nucleic acid hybridization on a paper-based platform using immobilized quantum dots (QDs) as donors in fluorescence resonance energy transfer (FRET). A nonenzymatic and reagentless means of signal enhancement for QD-FRET assays on paper substrates is based on the use of dry paper substrates for data acquisition. This approach offered at least a 10-fold higher assay sensitivity and at least a 10-fold lower limit of detection (LOD) as compared to hydrated paper substrates. The surface of paper was modified with imidazole groups to assemble a transduction interface that consisted of immobilized QD-probe oligonucleotide conjugates. Green-emitting QDs (gQDs) served as donors with Cy3 as an acceptor. A hybridization event that brought the Cy3 acceptor dye in close proximity to the surface of immobilized gQDs was responsible for a FRET-sensitized emission from the acceptor dye, which served as an analytical signal. A hand-held UV lamp was used as an excitation source and ratiometric analysis using an iPad camera was possible by a relative intensity analysis of the red (Cy3 photoluminescence (PL)) and green (gQD PL) color channels of the digital camera. For digital imaging using an iPad camera, the LOD of the assay in a sandwich format was 450 fmol with a dynamic range spanning 2 orders of magnitude, while an epifluorescence microscope detection platform offered a LOD of 30 fmol and a dynamic range spanning 3 orders of magnitude. The selectivity of the hybridization assay was demonstrated by detection of a single nucleotide polymorphism at a contrast ratio of 60:1. This work provides an
Energy Technology Data Exchange (ETDEWEB)
Kılıç, Bayram, E-mail: bkilic@yalova.edu.tr, E-mail: kbayramkilic@gmail.com [Department of Energy Systems Engineering, Faculty of Engineering, Yalova University, 77100 Yalova (Turkey); Telli, Hakan; Başaran, Ali; Pirge, Gursev [Turkish Air Force Academy, Institute of Aeronautics and Space Technologies, Istanbul (Turkey); Tüzemen, Sebahattin [Department of Physics, Faculty of Science, Ataturk University, Erzurum (Turkey)
2015-04-07
Dye sensitized solar cells (DSSCs) with an innovative design involving controlled-morphology vertically aligned (VA) ZnO nanowires within mesoporous TiO{sub 2} structures with ultrahigh surface area for implementation as photoanodes are herein reported. Although TiO{sub 2} nanostructures exhibit excellent power conversion efficiency, the electron transport rate is low owing to low electron mobility. To overcome this, ZnO nanowires with high electron mobility have been investigated as potential candidates for photoanodes. However, the power conversion efficiency of ZnO nanowires is still lower than that of TiO{sub 2} owing to their low internal surface area. Consequently, in this work, vertical growth of ZnO nanowires within mesoporous TiO{sub 2} structures is carried out to increase their solar power conversion efficiency. The photovoltaic performance of solar cells using ZnO nanowires, mesoporous TiO{sub 2}, and TiO{sub 2}/ZnO hybrid structures are compared. The VA TiO{sub 2}/ZnO hybrid structures are found to provide direct electron transfer compared with the tortuous pathway of zero-dimensional nanostructures, resulting in an increased conversion efficiency. It is demonstrated that the light scattering of the photoanode film is increased and electron recombination is decreased when an appropriate amount of mesoporous TiO{sub 2} is used as a substrate for ZnO nanowires. The DSSC fabricated with the TiO{sub 2}/ZnO hybrid photoanode prepared with 15.8 wt. % TiO{sub 2} showed the highest conversion efficiency of 7.30%, approximately 5%, 18%, and 40% higher than that of DSSCs fabricated with 3.99 wt. % TiO{sub 2}, pure TiO{sub 2}, and pure ZnO photoanodes, respectively.
Jeans instability in a quantum dusty magnetoplasma
International Nuclear Information System (INIS)
Salimullah, M.; Jamil, M.; Shah, H. A.; Murtaza, G.
2009-01-01
Jeans instability in a homogeneous cold quantum dusty plasma in the presence of the ambient magnetic field and the quantum effect arising through the Bohm potential has been examined using the quantum magnetohydrodynamic model. It is found that the Jeans instability is significantly reduced by the presence of the dust-lower-hybrid wave and the ion quantum effect. The minimum wavenumber for Jeans stability depends clearly on ion quantum effect and the dust-lower-hybrid frequency also.
International Nuclear Information System (INIS)
Hua, Mengjuan; Wang, Chengquan; Qian, Jing; Wang, Kan; Yang, Zhenting; Liu, Qian; Mao, Hanping; Wang, Kun
2015-01-01
We herein proposed a simple and effective strategy for preparing graphene quantum dots (GQDs)-based core-satellite hybrid spheres and further explored the feasibility of using such spheres as the ratiometric fluorescence probe for the visual determination of Hg 2+ . The red-emitting CdTe QDs were firstly entrapped in the silica nanosphere to reduce their toxicity and improve their photo and chemical stabilities, thus providing a built-in correction for environmental effects, while the GQDs possessing good biocompatibility and low toxicity were electrostatic self-assembly on the silica surface acting as reaction sites. Upon exposure to the increasing contents of Hg 2+ , the blue fluorescence of GQDs can be gradually quenched presumably due to facilitating nonradiative electron/hole recombination annihilation. With the embedded CdTe QDs as the internal standard, the variations of the tested solution display continuous fluorescence color changes from blue to red, which can be easily observed by the naked eye without any sophisticated instrumentations and specially equipped laboratories. This sensor exhibits high sensitivity and selectivity toward Hg 2+ in a broad linear range of 10 nM–22 μM with a low detection limit of 3.3 nM (S/N = 3), much lower than the allowable Hg 2+ contents in drinking water set by U.S. Environmental Protection Agency. This prototype ratiometric probe is of good simplicity, low toxicity, excellent stabilities, and thus potentially attractive for Hg 2+ quantification related biological systems. - Highlights: • A facile strategy for preparing GQDs based core-satellite hybrid spheres was reported. • Such spheres can be used as the ratiometric fluorescence probe for Hg 2+ detection. • The Hg 2+ content can be easily distinguished by the naked eye. • The sensor shows high sensitivity and selectivity toward Hg 2+ detection. • The ratiometric probe is of good simplicity, low toxicity, and excellent stability
Energy Technology Data Exchange (ETDEWEB)
Choi, Jin-Kyu; Dung, Mai Xuan; Jeong, Hyun-Dam, E-mail: hdjeong@chonnam.ac.kr
2014-11-14
We present a new material design concept, silicon quantum dot (Si QD) polymers, for which surface-functionalized Si QDs can be regarded as a large monomer in the polymers. As a prototypical example, vinyl-functionalized Si QDs, i.e., divinylbenzene-capped Si QDs (DVB-Si QDs) synthesized by adopting divinylbenzene (DVB) capping molecule to the hydride-terminated Si QD (H-Si QD) via Pt-catalyzed hydrosilylation was introduced and polymerized with a styrene monomer to yield Si QD–polystyrene (Si QD–PS) polymers. To demonstrate controllability of the content of Si QDs in the polymers as in conventional polymers, three Si QD content varied Si QD–PS polymers were systematically prepared, named as Si QD–PS-A, Si QD–PS-B, and Si QD–PS-C. It has been demonstrated that the content of the Si QDs in the Si QD–PS polymers was well controlled by the amount of the DVB-Si QD used, as found to be 3.8 wt% (Si QD–PS-A), 10.0 wt% (Si QD–PS-B), 20.0 wt% (Si QD–PS-A), and 37.4 wt% (DVB-Si QD), which was deduced from TGA results. Thin films of the Si QD–PS polymers and the freestanding DVB-Si QDs were successfully fabricated by a spin-coating method and it was found that the refractive index of the thin films dried at 40 °C was linearly increased as the content of the Si QD in the polymers was increased from 1.586 (0 wt%), to 1.590 (3.8 wt%), to 1.592 (10.0 wt%), to 1.592 (20.0 wt%), and to 1.614 (37.4 wt%). - Highlights: • A new material design concept, Si QD polymer, is presented. • Freestanding vinyl-functionalized Si QD was synthesized as a monomer for polymer. • Si QD–PS polymers were synthesized by polymerization of styrene with vinyl-Si QD. • Concentration of Si QD in the polymer was well controlled by amount of Si QD used. • Refractive index of polymer thin films linearly increased with concentration of Si QD.
International Nuclear Information System (INIS)
Choi, Jin-Kyu; Dung, Mai Xuan; Jeong, Hyun-Dam
2014-01-01
We present a new material design concept, silicon quantum dot (Si QD) polymers, for which surface-functionalized Si QDs can be regarded as a large monomer in the polymers. As a prototypical example, vinyl-functionalized Si QDs, i.e., divinylbenzene-capped Si QDs (DVB-Si QDs) synthesized by adopting divinylbenzene (DVB) capping molecule to the hydride-terminated Si QD (H-Si QD) via Pt-catalyzed hydrosilylation was introduced and polymerized with a styrene monomer to yield Si QD–polystyrene (Si QD–PS) polymers. To demonstrate controllability of the content of Si QDs in the polymers as in conventional polymers, three Si QD content varied Si QD–PS polymers were systematically prepared, named as Si QD–PS-A, Si QD–PS-B, and Si QD–PS-C. It has been demonstrated that the content of the Si QDs in the Si QD–PS polymers was well controlled by the amount of the DVB-Si QD used, as found to be 3.8 wt% (Si QD–PS-A), 10.0 wt% (Si QD–PS-B), 20.0 wt% (Si QD–PS-A), and 37.4 wt% (DVB-Si QD), which was deduced from TGA results. Thin films of the Si QD–PS polymers and the freestanding DVB-Si QDs were successfully fabricated by a spin-coating method and it was found that the refractive index of the thin films dried at 40 °C was linearly increased as the content of the Si QD in the polymers was increased from 1.586 (0 wt%), to 1.590 (3.8 wt%), to 1.592 (10.0 wt%), to 1.592 (20.0 wt%), and to 1.614 (37.4 wt%). - Highlights: • A new material design concept, Si QD polymer, is presented. • Freestanding vinyl-functionalized Si QD was synthesized as a monomer for polymer. • Si QD–PS polymers were synthesized by polymerization of styrene with vinyl-Si QD. • Concentration of Si QD in the polymer was well controlled by amount of Si QD used. • Refractive index of polymer thin films linearly increased with concentration of Si QD
Kong, Chang Sun; Haverty, Michael; Simka, Harsono; Shankar, Sadasivan; Rajan, Krishna
2017-09-01
We present a hybrid approach based on both machine learning and targeted ab-initio calculations to determine adhesion energies between dissimilar materials. The goals of this approach are to complement experimental and/or all ab-initio computational efforts, to identify promising materials rapidly and identify in a quantitative manner the relative contributions of the different material attributes affecting adhesion. Applications of the methodology to predict bulk modulus, yield strength, adhesion and wetting properties of copper (Cu) with other materials including metals, nitrides and oxides is discussed in this paper. In the machine learning component of this methodology, the parameters that were chosen can be roughly divided into four types: atomic and crystalline parameters (which are related to specific elements such as electronegativities, electron densities in Wigner-Seitz cells); bulk material properties (e.g. melting point), mechanical properties (e.g. modulus) and those representing atomic characteristics in ab-initio formalisms (e.g. pseudopotentials). The atomic parameters are defined over one dataset to determine property correlation with published experimental data. We then develop a semi-empirical model across multiple datasets to predict adhesion in material interfaces outside the original datasets. Since adhesion is between two materials, we appropriately use parameters which indicate differences between the elements that comprise the materials. These semi-empirical predictions agree reasonably with the trend in chemical work of adhesion predicted using ab-initio techniques and are used for fast materials screening. For the screened candidates, the ab-initio modeling component provides fundamental understanding of the chemical interactions at the interface, and explains the wetting thermodynamics of thin Cu layers on various substrates. Comparison against ultra-high vacuum (UHV) experiments for well-characterized Cu/Ta and Cu/α-Al2O3 interfaces is
Zhu, Wanlu; Duan, Jialong; Duan, Yanyan; Zhao, Yuanyuan; Tang, Qunwei
2017-11-01
Photovoltaics are promising solutions to energy crisis and environmental pollution problems. The dye-sensitized solar cells with mesoscopic structures have attracted growing interests because of zero emissions, easy fabrication, scalable materials and techniques, etc. However, the state-of-the-art dye-sensitized solar cells have narrow spectral absorption for photoelectric conversion and high electron-hole recombination rate under sunlight illumination. Therefore, it is a persistent object to make wide-spectral absorption and fast charge extraction solar cells for energy harvest in both solar and dark-light conditions. To address this issue, we present here experimental realization of a category of solar cells converting visible and near-infrared light into electricity by co-sensitizing photoanode with N719 dye and polyethylene glycol (PEG) modified carbon quantum dots (PEG-m-CQDs), arising from up-conversion and hole-transporting behaviors of PEG-m-CQDs as well as photofluorescence of green-emitting long persistence phosphors. The optimized solar cell yields maximized photoelectric conversion efficiencies of 9.89% and 25.81% under simulated sunlight (air mass 1.5, 100 mW cm-2) illumination and dark conditions, respectively. This work is far from optimization, but the physical proof-of-concept hybridized solar cell may markedly increase electricity generation time and total power output of photovoltaic platforms.
Heo, Jino; Hong, Chang-Ho; Lim, Jong-In; Yang, Hyung-Jin
2015-05-01
We propose an arbitrary controlled-unitary (CU) gate and a bidirectional quantum teleportation (BQTP) scheme. The proposed CU gate utilizes photonic qubits (photons) with cross-Kerr nonlinearities (XKNLs), X-homodyne detectors, and linear optical elements, and consists of the consecutive operation of a controlled-path (C-path) gate and a gathering-path (G-path) gate. It is almost deterministic and feasible with current technology when a strong coherent state and weak XKNLs are employed. Based on the CU gate, we present a BQTP scheme that simultaneously teleports two unknown photons between distant users by transmitting only one photon in a path-polarization intra-particle hybrid entangled state. Consequently, it is possible to experimentally implement BQTP with a certain success probability using the proposed CU gate. Project supported by the Ministry of Science, ICT&Future Planning, Korea, under the C-ITRC (Convergence Information Technology Research Center) Support program (NIPA-2013-H0301-13-3007) supervised by the National IT Industry Promotion Agency.
Jindal, Shikha; Giripunje, Sushama M.
2017-11-01
Quantum dots (QDs) are the suitable material for solar cell devices owing to its distinctive optical, electrical and electronic properties. Currently, the most efficient devices have employed the toxic QDs which cause destructive impact on environment. In the present article, we have used environment benign CuInS2 QDs as an acceptor material in bulk heterojunction device of P3HT and QDs. The energy level positions corroborated from UPS spectra substantiates the acceptor property of CuInS2. We scrutinized the hybrid solar cell by tailoring the acceptor content in active layer. The increased acceptor content intensifies the performance of device. The enhancement in photovoltaic parameters is mainly due to the fast dissociation and extraction of photogenerated excitons which occurs with the larger wt% of acceptor QDs. Current density-voltage characteristics describes the greater V oc and I sc in the 60 wt% CuInS2 QDs based solar cell as compared to the low wt% of QDs in the active layer.
Gao, Feng; Yang, Chuan-Lu; Wang, Mei-Shan; Ma, Xiao-Guang; Liu, Wen-Wang
2018-04-01
The feasibility of nanocomposites of cir-coronene graphene quantum dot (GQD) with phthalocyanine, tetrabenzoporphyrin, tetrabenzotriazaporphyrins, cis-tetrabenzodiazaporphyrins, tetrabenzomonoazaporphyrins and their Cu-metallated macrocycles as a sensitizer of dye-sensitized solar cells (DSSC) are investigated. Based on the first principles density functional theory (DFT), the geometrical structures of the separate GQD and 10 macrocycles, and their hybridized nanocomposites are fully optimized. The energy stabilities of the obtained structures are confirmed by harmonic frequency analysis. The optical absorptions of the optimized structures are calculated with time-dependent DFT. The feasibility of the nanocomposites as the sensitizer of DSSC is examined by the charge spatial separation, the electron transfer, the molecular orbital energy levels of the nanocomposites and the electrolyte, and the conduction band minimum of TiO2 electrode. The results demonstrate that all the nanocomposites have enhanced absorptions in the visible light range, and their molecular orbital energies satisfy the requirement of sensitizers. However, only two of the ten considered nanocomposites demonstrate significantly charge spatial separation. The GQD-Cu-TBP is identified as the most favorable candidate sensitizer of DSSC by the most enhanced in optical absorption, obvious charge spatial separation, suitable LUMO energy levels and driving force for electron transfer, and low recombination rate of electron and hole.
Hapuarachchi, Harini; Mallawaarachchi, Sudaraka; Hattori, Haroldo T.; Zhu, Weiren; Premaratne, Malin
2018-02-01
Recently, many have studied various configurations of metal nanoparticle-quantum dot (MNP-QD) hybrid molecules based on different metals and tunable parameters. In this paper, we aim to incite the interest in using MNP-QD nanohybrids, which possess sensing capabilities superior to those of the individual constituents, for sensing applications that rely on scattered light. When assessing whether a given MNP-QD configuration is suited for an application, sometimes it is hard to assess the pros and cons of a given configuration against other candidates. Here we propose a simple, elegant relative figure of merit (RFoM), which focuses on maximizing the scattered intensity and the refractive index sensitivity of the nanohybrid, to rank the suitability of viable MNP-QD configurations for a particular sensing application. We use the proposed RFoM to analyse the optical spectra of noble, transition, post transition and alkali metal based MNP-QD nanohybrids using the representative metals Au, Ag, Cu, Al and Na, adopting a generalized nonlocal optical response (GNOR) method based cavity QED approach. Based on our observations, we suggest how the usage of MNP-QD nanohybrids could improve the conventionally studied tumour targeting applications. Moreover, we propose potential substitutes for noble metals conventionally considered for MNP-QD nanohybrids.
Universal quantum computation by discontinuous quantum walk
International Nuclear Information System (INIS)
Underwood, Michael S.; Feder, David L.
2010-01-01
Quantum walks are the quantum-mechanical analog of random walks, in which a quantum ''walker'' evolves between initial and final states by traversing the edges of a graph, either in discrete steps from node to node or via continuous evolution under the Hamiltonian furnished by the adjacency matrix of the graph. We present a hybrid scheme for universal quantum computation in which a quantum walker takes discrete steps of continuous evolution. This ''discontinuous'' quantum walk employs perfect quantum-state transfer between two nodes of specific subgraphs chosen to implement a universal gate set, thereby ensuring unitary evolution without requiring the introduction of an ancillary coin space. The run time is linear in the number of simulated qubits and gates. The scheme allows multiple runs of the algorithm to be executed almost simultaneously by starting walkers one time step apart.
Scalable optical quantum computer
Energy Technology Data Exchange (ETDEWEB)
Manykin, E A; Mel' nichenko, E V [Institute for Superconductivity and Solid-State Physics, Russian Research Centre ' Kurchatov Institute' , Moscow (Russian Federation)
2014-12-31
A way of designing a scalable optical quantum computer based on the photon echo effect is proposed. Individual rare earth ions Pr{sup 3+}, regularly located in the lattice of the orthosilicate (Y{sub 2}SiO{sub 5}) crystal, are suggested to be used as optical qubits. Operations with qubits are performed using coherent and incoherent laser pulses. The operation protocol includes both the method of measurement-based quantum computations and the technique of optical computations. Modern hybrid photon echo protocols, which provide a sufficient quantum efficiency when reading recorded states, are considered as most promising for quantum computations and communications. (quantum computer)
Scalable optical quantum computer
International Nuclear Information System (INIS)
Manykin, E A; Mel'nichenko, E V
2014-01-01
A way of designing a scalable optical quantum computer based on the photon echo effect is proposed. Individual rare earth ions Pr 3+ , regularly located in the lattice of the orthosilicate (Y 2 SiO 5 ) crystal, are suggested to be used as optical qubits. Operations with qubits are performed using coherent and incoherent laser pulses. The operation protocol includes both the method of measurement-based quantum computations and the technique of optical computations. Modern hybrid photon echo protocols, which provide a sufficient quantum efficiency when reading recorded states, are considered as most promising for quantum computations and communications. (quantum computer)
Kaganovich, I D; Startsev, E
2005-01-01
Ion-atom ionization cross sections are needed in many applications employing the propagation of fast ions through matter. When experimental data or full-scale theoretical calculations are non-existent, approximate methods must be used. The most robust and easy-to-use approximations include the Born approximation of quantum mechanics and the quasi-classical approach utilizing classical mechanics together with the Bohr-Sommerfeld quantization rule.* The simplest method to extend the validity of both approaches is to combine them, i.e., use the two different approaches but only for the regions of impact parameters in which they are valid, and sum the results to obtain the total cross section. We have recently investigated theoretically and experimentally the stripping of more than 18 different pairs of projectile and target atoms in the range of 3-38 MeV/amu to study the range of validity of various approximations. The results of the modified approach agree better with the experimental data than either the Born ...
Energy Technology Data Exchange (ETDEWEB)
Wang, Wei [School of Physics and Optoelectronic Engineering, Nanjing University of Information Science and Technology, Nanjing 210044 (China); Ni, Yaru; Xu, Zhongzi [College of Materials Science and Engineering, Nanjing Tech University, Nanjing 210009 (China)
2015-02-15
Highlights: • CQDs were uniformly deposited on high-reactive TiO{sub 2} by a one-pot method. • CQDs can use a wide range of solar spectrum efficiently for photocatalysis. • TiO{sub 2} facets are not affected and the total photocatalytic activity was improved. - Abstract: High-reactive facets dominated anatase TiO{sub 2} is of great significance to solve environment and energy challenges. Maintaining the pristine structure and improving the photocatalytic activity of TiO{sub 2} still need innovation work by employing different modification processes. Here, carbon quantum dots (CQDs) were employed to modify TiO{sub 2} with exposed {0 0 1}, {1 0 1}, and {0 1 0} facets by a one-pot hydrothermal method. Results indicate that CQDs can disperse uniformly on TiO{sub 2} surface, and the high-reactive facets are maintained perfectly. The introduced CQDs can both enhance the light absorption and suppress photogenerated electron-hole’s recombination. Proper amount of introduced CQDs can both significantly enhance the photocatalytic activities, which are very stable, under the UV and visible light irradiation Corresponding photocatalytic mechanisms are also discussed in the present work.
Programmable architecture for quantum computing
Chen, J.; Wang, L.; Charbon, E.; Wang, B.
2013-01-01
A programmable architecture called “quantum FPGA (field-programmable gate array)” (QFPGA) is presented for quantum computing, which is a hybrid model combining the advantages of the qubus system and the measurement-based quantum computation. There are two kinds of buses in QFPGA, the local bus and
Fu, Weifei; Wang, Ling; Zhang, Yanfang; Ma, Ruisong; Zuo, Lijian; Mai, Jiangquan; Lau, Tsz-Ki; Du, Shixuan; Lu, Xinhui; Shi, Minmin; Li, Hanying; Chen, Hongzheng
2014-11-12
Achieving superior solar cell performance based on the colloidal nanocrystals remains challenging due to their complex surface composition. Much attention has been devoted to the development of effective surface modification strategies to enhance electronic coupling between the nanocrystals to promote charge carrier transport. Herein, we aim to attach benzenedithiol ligands onto the surface of CdSe nanocrystals in the "face-on" geometry to minimize the nanocrystal-nanocrystal or polymer-nanocrystal distance. Furthermore, the "electroactive" π-orbitals of the benzenedithiol are expected to further enhance the electronic coupling, which facilitates charge carrier dissociation and transport. The electron mobility of CdSe QD films was improved 20 times by tuning the ligand orientation, and high performance poly[2,6-(4,4-bis(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']-dithiophene)-alt-4,7-(2,1,3-benzothiadiazole)] (PCPDTBT):CdSe nanocrystal hybrid solar cells were also achieved, showing a highest power conversion efficiency of 4.18%. This research could open up a new pathway to improve further the performance of colloidal nanocrystal based solar cells.
Ahmed, Syed Rahin; Mogus, Jack; Chand, Rohit; Nagy, Eva; Neethirajan, Suresh
2018-04-30
An optoelectronic sensor is a rapid diagnostic tool that allows for an accurate, reliable, field-portable, low-cost device for practical applications. In this study, template-free In situ gold nanobundles (Au NBs) were fabricated on an electrode for optoelectronic sensing of fowl adenoviruses (FAdVs). Au NB film was fabricated on carbon electrodes working area using L(+) ascorbic acid, gold chroloauric acid and poly-l-lysine (PLL) through modified layer-by-layer (LbL) method. A scanning electron microscopic (SEM) image of the Au NBs revealed a NB-shaped Au structure with many kinks on its surface, which allow local electric field enhancement through light-matter interaction with graphene quantum dots (GQDs). Here, GQDs were synthesized through an autoclave-assisted method. Characterization experiments revealed blue-emissive, well-dispersed GQDs that were 2-3nm in size with the fluorescence emission peak of GQDs located at 405nm. Both Au NBs and GQDs were conjugated with target FAdVs specific antibodies that bring them close to each other with the addition of target FAdVs through antibody-antigen interaction. At close proximity, light-matter interaction between Au NBs and QDs produces a local electric signal enhancement under Ultraviolet-visible (UV-visible) light irradiation that allows the detection of very low concentrations of target virus even in complex biological media. A proposed optoelectronic sensor showed a linear relationship between the target FAdVs and the electric signal up to 10 Plaque forming unit (PFU)/mL with a limit of detection (LOD) of 8.75 PFU/mL. The proposed sensing strategy was 100 times more sensitive than conventional ELISA method. Copyright © 2017 Elsevier B.V. All rights reserved.
Energy Technology Data Exchange (ETDEWEB)
Hua, Mengjuan [Key Laboratory of Modern Agriculture Equipment and Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013 (China); Wang, Chengquan [School of Food and Biological Engineering, Jiangsu University, Zhenjiang 212013 (China); Qian, Jing, E-mail: qianj@ujs.edu.cn [Key Laboratory of Modern Agriculture Equipment and Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013 (China); Wang, Kan; Yang, Zhenting; Liu, Qian; Mao, Hanping [Key Laboratory of Modern Agriculture Equipment and Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013 (China); Wang, Kun, E-mail: wangkun@ujs.edu.cn [Key Laboratory of Modern Agriculture Equipment and Technology, School of Chemistry and Chemical Engineering, Jiangsu University, Zhenjiang 212013 (China)
2015-08-12
We herein proposed a simple and effective strategy for preparing graphene quantum dots (GQDs)-based core-satellite hybrid spheres and further explored the feasibility of using such spheres as the ratiometric fluorescence probe for the visual determination of Hg{sup 2+}. The red-emitting CdTe QDs were firstly entrapped in the silica nanosphere to reduce their toxicity and improve their photo and chemical stabilities, thus providing a built-in correction for environmental effects, while the GQDs possessing good biocompatibility and low toxicity were electrostatic self-assembly on the silica surface acting as reaction sites. Upon exposure to the increasing contents of Hg{sup 2+}, the blue fluorescence of GQDs can be gradually quenched presumably due to facilitating nonradiative electron/hole recombination annihilation. With the embedded CdTe QDs as the internal standard, the variations of the tested solution display continuous fluorescence color changes from blue to red, which can be easily observed by the naked eye without any sophisticated instrumentations and specially equipped laboratories. This sensor exhibits high sensitivity and selectivity toward Hg{sup 2+} in a broad linear range of 10 nM–22 μM with a low detection limit of 3.3 nM (S/N = 3), much lower than the allowable Hg{sup 2+} contents in drinking water set by U.S. Environmental Protection Agency. This prototype ratiometric probe is of good simplicity, low toxicity, excellent stabilities, and thus potentially attractive for Hg{sup 2+} quantification related biological systems. - Highlights: • A facile strategy for preparing GQDs based core-satellite hybrid spheres was reported. • Such spheres can be used as the ratiometric fluorescence probe for Hg{sup 2+} detection. • The Hg{sup 2+} content can be easily distinguished by the naked eye. • The sensor shows high sensitivity and selectivity toward Hg{sup 2+} detection. • The ratiometric probe is of good simplicity, low toxicity, and
Xu, Yongjie; Li, Xinyu; Hu, Guanghui; Wu, Ting; Luo, Yi; Sun, Lang; Tang, Tao; Wen, Jianfeng; Wang, Heng; Li, Ming
2017-11-01
Nitrogen-enriched graphene was fabricated via a facile strategy. Graphene oxide (GO) nanosheets and graphene oxide quantum dots (GQDs) were used as a structure-directing agent and in situ activating agent, respectively, after photoreduction under NH3 atmosphere. The combination of photoreduction and NH3 not only reduced GO and GQD composites (GO/GQDs) within a shorter duration but also doped a high level of nitrogen on the composites (NrGO/GQDs). The nitrogen content of NrGO/GQDs reached as high as 18.86 at% within 5 min of irradiation. Benefiting from the nitrogen-enriched GO/GQDs hybrid structure, GQDs effectively prevent the agglomeration of GO sheets and increased the numbers of ion channels in the material. Meanwhile, the high levels of nitrogen improved electrical conductivity and strengthened the binding energy between GQD and GO sheets. Compared with reduced GO and low nitrogen-doped reduced GO, NrGO/GQD electrodes exhibited better electrochemical characteristics with a high specific capacitance of 344 F g-1 at a current density of 0.25 A g-1. Moreover, the NrGO/GQD electrodes exhibited 82% capacitance retention after 3000 cycles at a current density of 0.8 A g-1 in 6 M KOH electrolyte. More importantly, the NrGO/GQD electrodes deliver a high energy density of 43 Wh kg-1 at a power density of 417 W kg-1 in 1 M Li2SO4 electrolyte. The nitrogen-doped graphene and corresponding supercapacitor presented in this study are novel materials with potential applications in advanced energy storage systems.
Tirler, Andreas O; Hofer, Thomas S
2014-11-13
This investigation presents the characterization of structural and dynamical properties of uranyl tricarbonate in aqueous solution employing an extended hybrid quantum mechanical/molecular mechanical (QM/MM) approach. It is shown that the inclusion of explicit solvent molecules in the quantum chemical treatment is essential to mimic the complex interaction occurring in an aqueous environment. Thus, in contrast to gas phase cluster calculations on a quantum chemical level proposing a 6-fold coordination of the three carbonates, the QMCF MD simulation proposes a 5-fold coordination. An extensive comparison of the simulation results to structural and dynamical data available in the literature was found to be in excellent agreement. Furthermore, this work is the first theoretical study on a quantum chemical level of theory able to observe the conversion of carbonate (CO₃²⁻) to bicarbonate (HCO₃⁻) in the equatorial coordination sphere of the uranyl ion. From a comparison of the free energy ΔG values for the unprotonated educt [UO₂(CO₃)₃]⁴⁻ and the protonated [UO₂(CO₃)₂(HCO₃)]³⁻, it could be concluded that the reaction equilibrium is strongly shifted toward the product state confirming the benignity for the observed protonation reaction. Structural properties and the three-dimensional arrangement of carbonate ligands were analyzed via pair-, three-body, and angular distributions, the dynamical properties were evaluated by hydrogen-bond correlation functions and vibrational power spectra.
DEFF Research Database (Denmark)
Aidas, Kestutis; Olsen, Jógvan Magnus Haugaard; Kongsted, Jacob
2013-01-01
Attempting to unravel mechanisms in optical probing of proteins, we have performed pilot calculations of two cationic chromophores—acridine yellow and proflavin—located at different binding sites within human serum albumin, including the two primary drug binding sites as well as a heme binding site....... The computational scheme adopted involves classical molecular dynamics simulations of the ligands bound to the protein and subsequent linear response polarizable embedding density functional theory calculations of the excitation energies. A polarizable embedding potential consisting of point charges fitted...
Nucleic acid reactivity : challenges for next-generation semiempirical quantum models
Huang, Ming; Giese, Timothy J.; York, Darrin M.
2015-01-01
Semiempirical quantum models are routinely used to study mechanisms of RNA catalysis and phosphoryl transfer reactions using combined quantum mechanical/molecular mechanical methods. Herein, we provide a broad assessment of the performance of existing semiempirical quantum models to describe nucleic acid structure and reactivity in order to quantify their limitations and guide the development of next-generation quantum models with improved accuracy. Neglect of diatomic diffierential overlap (...
National Research Council Canada - National Science Library
Agarwal, G. S
2013-01-01
.... Focusing on applications of quantum optics, the textbook covers recent developments such as engineering of quantum states, quantum optics on a chip, nano-mechanical mirrors, quantum entanglement...
Super-activating Quantum Memory with Entanglement
Guan, Ji; Feng, Yuan; Ying, Mingsheng
2017-01-01
Noiseless subsystems were proved to be an efficient and faithful approach to preserve fragile information against decoherence in quantum information processing and quantum computation. They were employed to design a general (hybrid) quantum memory cell model that can store both quantum and classical information. In this Letter, we find an interesting new phenomenon that the purely classical memory cell can be super-activated to preserve quantum states, whereas the null memory cell can only be...
Esposito, A.; Polosa, A.D.
2016-01-01
We propose a new interpretation of the neutral and charged X, Z exotic hadron resonances. Hybridized-tetraquarks are neither purely compact tetraquark states nor bound or loosely bound molecules. The latter would require a negative or zero binding energy whose counterpart in h-tetraquarks is a positive quantity. The formation mechanism of this new class of hadrons is inspired by that of Feshbach metastable states in atomic physics. The recent claim of an exotic resonance in the Bs pi+- channel by the D0 collaboration and the negative result presented subsequently by the LHCb collaboration are understood in this scheme, together with a considerable portion of available data on X, Z particles. Considerations on a state with the same quantum numbers as the X(5568) are also made.
Yuan, Jipei; Guo, Weiwei; Wang, Erkang
2008-02-15
In this paper, we attempt to construct a simple and sensitive detection method for both phenolic compounds and hydrogen peroxide, with the successful combination of the unique property of quantum dots and the specificity of enzymatic reactions. In the presence of H2O2 and horseradish peroxidase, phenolic compounds can quench quantum dots' photoluminescence efficiently, and the extent of quenching is severalfold to more than 100-fold increase. Quinone intermediates produced from the enzymatic catalyzed oxidation of phenolic compounds were believed to play the main role in the photoluminescence quenching. Using a quantum dots-enzyme system, the detection limits for phenolic compounds and hydrogen peroxide were detected to be approximately 10(-7) mol L(-1). The coupling of efficient quenching of quantum dot photoluminescence by quinone and the effective enzymatic reactions make this a simple and sensitive method for phenolic compound detection and great potential in the development of H2O2 biosensors for various analytes.
Quantum Transduction with Adaptive Control
Zhang, Mengzhen; Zou, Chang-Ling; Jiang, Liang
2018-01-01
Quantum transducers play a crucial role in hybrid quantum networks. A good quantum transducer can faithfully convert quantum signals from one mode to another with minimum decoherence. Most investigations of quantum transduction are based on the protocol of direct mode conversion. However, the direct protocol requires the matching condition, which in practice is not always feasible. Here we propose an adaptive protocol for quantum transducers, which can convert quantum signals without requiring the matching condition. The adaptive protocol only consists of Gaussian operations, feasible in various physical platforms. Moreover, we show that the adaptive protocol can be robust against imperfections associated with finite squeezing, thermal noise, and homodyne detection, and it can be implemented to realize quantum state transfer between microwave and optical modes.
Quantum Transduction with Adaptive Control.
Zhang, Mengzhen; Zou, Chang-Ling; Jiang, Liang
2018-01-12
Quantum transducers play a crucial role in hybrid quantum networks. A good quantum transducer can faithfully convert quantum signals from one mode to another with minimum decoherence. Most investigations of quantum transduction are based on the protocol of direct mode conversion. However, the direct protocol requires the matching condition, which in practice is not always feasible. Here we propose an adaptive protocol for quantum transducers, which can convert quantum signals without requiring the matching condition. The adaptive protocol only consists of Gaussian operations, feasible in various physical platforms. Moreover, we show that the adaptive protocol can be robust against imperfections associated with finite squeezing, thermal noise, and homodyne detection, and it can be implemented to realize quantum state transfer between microwave and optical modes.
Quantum Erasure: Quantum Interference Revisited
Walborn, Stephen P.; Cunha, Marcelo O. Terra; Pádua, Sebastião; Monken, Carlos H.
2005-01-01
Recent experiments in quantum optics have shed light on the foundations of quantum physics. Quantum erasers - modified quantum interference experiments - show that quantum entanglement is responsible for the complementarity principle.
Quantum control using genetic algorithms in quantum communication: superdense coding
International Nuclear Information System (INIS)
Domínguez-Serna, Francisco; Rojas, Fernando
2015-01-01
We present a physical example model of how Quantum Control with genetic algorithms is applied to implement the quantum superdense code protocol. We studied a model consisting of two quantum dots with an electron with spin, including spin-orbit interaction. The electron and the spin get hybridized with the site acquiring two degrees of freedom, spin and charge. The system has tunneling and site energies as time dependent control parameters that are optimized by means of genetic algorithms to prepare a hybrid Bell-like state used as a transmission channel. This state is transformed to obtain any state of the four Bell basis as required by superdense protocol to transmit two bits of classical information. The control process protocol is equivalent to implement one of the quantum gates in the charge subsystem. Fidelities larger than 99.5% are achieved for the hybrid entangled state preparation and the superdense operations. (paper)
Quantum dynamical entropy revisited
International Nuclear Information System (INIS)
Hudetz, T.
1996-10-01
We define a new quantum dynamical entropy, which is a 'hybrid' of the closely related, physically oriented entropy introduced by Alicki and Fannes in 1994, and of the mathematically well-developed, single-argument entropy introduced by Connes, Narnhofer and Thirring in 1987. We show that this new quantum dynamical entropy has many properties similar to the ones of the Alicki-Fannes entropy, and also inherits some additional properties from the CNT entropy. In particular, the 'hybrid' entropy interpolates between the two different ways in which both the AF and the CNT entropy of the shift automorphism on the quantum spin chain agree with the usual quantum entropy density, resulting in even better agreement. Also, the new quantum dynamical entropy generalizes the classical dynamical entropy of Kolmogorov and Sinai in the same way as does the AF entropy. Finally, we estimate the 'hybrid' entropy both for the Powers-Price shift systems and for the noncommutative Arnold map on the irrational rotation C * -algebra, leaving some interesting open problems. (author)
Cai, Xing-Wei; Zhao, Yu-Yuan; Li, Hong; Huang, Cui-Ping; Zhou, Zhen
2018-06-01
With the flourishing development of emitting materials, tremendous technological progress has been accomplished. However, they still face great challenges in convenient economical environmental-friendly large-scale commercial production. Herein we designed this organic-inorganic hybrid lead-free compound, an emerging class of high-efficiency emitting materials, [(C10H16N)2][MnBr4] (1), which emits intense greenish photoluminescence with a high emissive quantum yields of 72.26%, was prepared through the convenient economical solution method. What's more, compared with rare earth fluorescent materials (especially green-emitting Tb), Mn material is rich in natural resources and low commercial cost, which would possess an increasingly predominant advantage in the preparation of luminescent materials. Additionally, the exceptional thermal stability as well as the low-cost/convenient preparation process makes crystal 1 with the large size of more than 1 cm to be an ideal technologically important green-emitting material and it would open up a new route towards the commercialization process of lead-free/rare earth-free hybrid emitting materials in display and sensing.
Systematic Quantum Mechanical Region Determination in QM/MM Simulation.
Karelina, Maria; Kulik, Heather J
2017-02-14
Hybrid quantum mechanical-molecular mechanical (QM/MM) simulations are widely used in enzyme simulation. Over ten convergence studies of QM/MM methods have revealed over the past several years that key energetic and structural properties approach asymptotic limits with only very large (ca. 500-1000 atom) QM regions. This slow convergence has been observed to be due in part to significant charge transfer between the core active site and the surrounding protein environment, which cannot be addressed by improvement of MM force fields or the embedding method employed within QM/MM. Given this slow convergence, it becomes essential to identify strategies for the most atom-economical determination of optimal QM regions and to gain insight into the crucial interactions captured only in large QM regions. Here, we extend and develop two methods for quantitative determination of QM regions. First, in the charge shift analysis (CSA) method, we probe the reorganization of electron density when core active site residues are removed completely, as determined by large-QM region QM/MM calculations. Second, we introduce the highly parallelizable Fukui shift analysis (FSA), which identifies how core/substrate frontier states are altered by the presence of an additional QM residue in smaller initial QM regions. We demonstrate that the FSA and CSA approaches are complementary and consistent on three test case enzymes: catechol O-methyltransferase, cytochrome P450cam, and hen eggwhite lysozyme. We also introduce validation strategies and test the sensitivities of the two methods to geometric structure, basis set size, and electronic structure methodology. Both methods represent promising approaches for the systematic, unbiased determination of quantum mechanical effects in enzymes and large systems that necessitate multiscale modeling.
National Research Council Canada - National Science Library
Agarwal, G. S
2013-01-01
..., quantum metrology, spin squeezing, control of decoherence and many other key topics. Readers are guided through the principles of quantum optics and their uses in a wide variety of areas including quantum information science and quantum mechanics...
HYBRIDIZATION AND MOLECULAR GEOMETRY: A NUMBER GAME
African Journals Online (AJOL)
Temechegn
This article is not emphasizing the theory behind the hybridization, but only on how to ... The new orbitals have the same total electron capacity .... the quantum mechanics and from a theory of paramagnetic susceptibility to the structure.
Directory of Open Access Journals (Sweden)
A. Jamshidi
2015-01-01
Full Text Available Colloidal Mn-doped ZnSe/CdS core/shell quantum dots (QDs are synthesized for the first time and employed as a strategy to boost the power conversion efficiency of quantum dot sensitized solar cells. By using Mn-doping as a band gap engineering tool for core/shell QDs an effective improvement of absorption spectra could be obtained. The mid-states generated by a proper Mn content alleviate carrier separation and enhance the electron injection rate, thus facilitating electron transport to the TiO2 substrate. It is demonstrated that a device constructed with 0.25% Mn-doped ZnSe/CdS leads to an enhancement of the electron injection rate and power conversion efficiency by 4 times and 1.3, respectively.
Quantum Instantons and Quantum Chaos
Jirari, H.; Kröger, H.; Luo, X. Q.; Moriarty, K. J. M.; Rubin, S. G.
1999-01-01
Based on a closed form expression for the path integral of quantum transition amplitudes, we suggest rigorous definitions of both, quantum instantons and quantum chaos. As an example we compute the quantum instanton of the double well potential.
Energy Technology Data Exchange (ETDEWEB)
Rudno-Rudzinski, Wojciech; Syperek, Marcin; Marynski, Aleksander; Andrzejewski, Janusz; Misiewicz, Jan; Sek, Grzegorz [Faculty of Fundamental Problems of Technology, Department of Experimental Physics, Wroclaw University of Science and Technology, Wroclaw (Poland); Bauer, Sven; Sichkovskyi, Vitalii I.; Reithmaier, Johann P. [Institute of Nanostructure Technology and Analytics, CINSaT, University of Kassel (Germany); Schowalter, Marco; Gerken, Beeke; Rosenauer, Andreas [Institute of Solid State Physics, Universitaet Bremen (Germany)
2018-02-15
The molecular beam epitaxy grown structures are investigated, comprising of InGaAs quantum wells (QW) separated by a thin InGaAlAs barrier from InAs quantum dots (QDs), emitting at 1.55 μm, grown on an InP substrate. To control the coupling between QW and QD parts the thickness of the barrier is changed, which commands the wave function overlap. The tuning of that parameter allows for the study of the influence of the QW potential on the energy structure of states and their wave functions in QDs, changing from an uncoupled system, where the optical response is just a sum of responses from two isolated elements, to a strongly quantum mechanically coupled system, exhibiting mixed 2D-0D characteristics. The changes of the energy structure that are deduced from the photoreflectance and photoluminescence spectroscopy results, supported by 8-band k . p modeling, explain the measured differences in the photoluminescence decay times between samples with different barrier thicknesses. (copyright 2017 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)
DEFF Research Database (Denmark)
Kopylov, Oleksii; Huck, Alexander; Shirazi, Roza
2013-01-01
We demonstrate light color conversion in patterned InGaN light-emitting diodes (LEDs), which is enhanced via nonradiative exciton resonant energy transfer (RET) from the electrically driven diode to colloidal semiconductor nanocrystals (NCs). Patterning of the diode is essential for the coupling...... between a quantum well (QW) and NCs, because the distance between the QW and NCs is a main and very critical factor of RET. Moreover, a proper design of the pattern can enhance light extraction....
International Nuclear Information System (INIS)
Xiang Guo-Yong; Guo Guang-Can
2013-01-01
The statistical error is ineluctable in any measurement. Quantum techniques, especially with the development of quantum information, can help us squeeze the statistical error and enhance the precision of measurement. In a quantum system, there are some quantum parameters, such as the quantum state, quantum operator, and quantum dimension, which have no classical counterparts. So quantum metrology deals with not only the traditional parameters, but also the quantum parameters. Quantum metrology includes two important parts: measuring the physical parameters with a precision beating the classical physics limit and measuring the quantum parameters precisely. In this review, we will introduce how quantum characters (e.g., squeezed state and quantum entanglement) yield a higher precision, what the research areas are scientists most interesting in, and what the development status of quantum metrology and its perspectives are. (topical review - quantum information)
Quantum Distinction: Quantum Distinctiones!
Zeps, Dainis
2009-01-01
10 pages; How many distinctions, in Latin, quantum distinctiones. We suggest approach of anthropic principle based on anthropic reference system which should be applied equally both in theoretical physics and in mathematics. We come to principle that within reference system of life subject of mathematics (that of thinking) should be equated with subject of physics (that of nature). For this reason we enter notions of series of distinctions, quantum distinction, and argue that quantum distinct...
Quantum simulations with photons and polaritons merging quantum optics with condensed matter physics
2017-01-01
This book reviews progress towards quantum simulators based on photonic and hybrid light-matter systems, covering theoretical proposals and recent experimental work. Quantum simulators are specially designed quantum computers. Their main aim is to simulate and understand complex and inaccessible quantum many-body phenomena found or predicted in condensed matter physics, materials science and exotic quantum field theories. Applications will include the engineering of smart materials, robust optical or electronic circuits, deciphering quantum chemistry and even the design of drugs. Technological developments in the fields of interfacing light and matter, especially in many-body quantum optics, have motivated recent proposals for quantum simulators based on strongly correlated photons and polaritons generated in hybrid light-matter systems. The latter have complementary strengths to cold atom and ion based simulators and they can probe for example out of equilibrium phenomena in a natural driven-dissipative sett...
Li, Yanna; Gessner, Manuel; Li, Weidong; Smerzi, Augusto
2018-02-01
The controlled generation and identification of quantum correlations, usually encoded in either qubits or continuous degrees of freedom, builds the foundation of quantum information science. Recently, more sophisticated approaches, involving a combination of two distinct degrees of freedom, have been proposed to improve on the traditional strategies. Hyperentanglement describes simultaneous entanglement in more than one distinct degree of freedom, whereas hybrid entanglement refers to entanglement shared between a discrete and a continuous degree of freedom. In this work we propose a scheme that allows us to combine the two approaches, and to extend them to the strongest form of quantum correlations. Specifically, we show how two identical, initially separated particles can be manipulated to produce Bell nonlocality among their spins, among their momenta, as well as across their spins and momenta. We discuss possible experimental realizations with atomic and photonic systems.
International Nuclear Information System (INIS)
Deus, Fernanda; Continetino, Mucio
2011-01-01
Full text. In this work we study the time dependent transport in interacting quantum dot. This is a zero-dimensional nano structure system which has quantized electronic states. In our purpose, we are interested in studying such system in a Coulomb blockade regime where a mean-field treatment of the electronic correlations are appropriate. The quantum dot is described by an Anderson type of Hamiltonian where the hybridization term arises from the contact with the leads. We consider a time dependence of both the energy of the localized state in the quantum dot and of the hybridization-like term. These time dependent parameters, under certain conditions, induce a current in the quantum dot even in the absence of difference on the chemical potential of the leads. The approach to this non-equilibrium problem requires the use of a Keldysh formalism. We calculate the non- equilibrium Green's functions and obtain results for the average (equilibrium term) and the non-equilibrium values of the electronic occupation number in the dot. we consider the possibility of a magnetic solution, with different values for the average up and down spins in the quantum dot. Our results allow to obtain, for instance, the tunneling current through the dot. The magnetic nature of the dot, for a certain range of parameters should give rise also to an induced spin current through the dot
International Nuclear Information System (INIS)
Takeoka, Masahiro; Fujiwara, Mikio; Mizuno, Jun; Sasaki, Masahide
2004-01-01
Quantum-information theory predicts that when the transmission resource is doubled in quantum channels, the amount of information transmitted can be increased more than twice by quantum-channel coding technique, whereas the increase is at most twice in classical information theory. This remarkable feature, the superadditive quantum-coding gain, can be implemented by appropriate choices of code words and corresponding quantum decoding which requires a collective quantum measurement. Recently, an experimental demonstration was reported [M. Fujiwara et al., Phys. Rev. Lett. 90, 167906 (2003)]. The purpose of this paper is to describe our experiment in detail. Particularly, a design strategy of quantum-collective decoding in physical quantum circuits is emphasized. We also address the practical implication of the gain on communication performance by introducing the quantum-classical hybrid coding scheme. We show how the superadditive quantum-coding gain, even in a small code length, can boost the communication performance of conventional coding techniques
Wisby, I. S.; de Graaf, S. E.; Gwilliam, R.; Adamyan, A.; Kubatkin, S. E.; Meeson, P. J.; Tzalenchuk, A. Ya.; Lindstrom, T.
Rare-earth doped crystals interfaced with superconducting quantum circuitry are an attractive platform for quantum memory and transducer applications. Here we present a detailed characterization of a locally implanted Gd3+ in Al2O3 system coupled to a superconducting micro-resonator, by performing angular dependent micro-electron-spin-resonance (micro-ESR) measurements at mK temperatures. The device is fabricated using a hard Si3N4 mask to facilitate a local ion-implantation technique for precision control of the dopant location. The technique is found not to degrade the internal quality factor of the resonators which remains above 105 (1). We find the measured angular dependence of the micro-ESR spectra to be in excellent agreement with the modelled Hamiltonian, supporting the conclusion that the dopant ions are successfully integrated into their relevant lattice sites whilst maintaining crystalline symmetries. Furthermore, we observe clear contributions from individual microwave field components of our micro-resonator, emphasising the need for controllable local implantation. 1 Wisby et al. Appl. Phys. Lett. 105, 102601 (2014)
Quantum walks, quantum gates, and quantum computers
International Nuclear Information System (INIS)
Hines, Andrew P.; Stamp, P. C. E.
2007-01-01
The physics of quantum walks on graphs is formulated in Hamiltonian language, both for simple quantum walks and for composite walks, where extra discrete degrees of freedom live at each node of the graph. It is shown how to map between quantum walk Hamiltonians and Hamiltonians for qubit systems and quantum circuits; this is done for both single-excitation and multiexcitation encodings. Specific examples of spin chains, as well as static and dynamic systems of qubits, are mapped to quantum walks, and walks on hyperlattices and hypercubes are mapped to various gate systems. We also show how to map a quantum circuit performing the quantum Fourier transform, the key element of Shor's algorithm, to a quantum walk system doing the same. The results herein are an essential preliminary to a Hamiltonian formulation of quantum walks in which coupling to a dynamic quantum environment is included
Le Gouët, Jean-Louis; Moiseev, Sergey
2012-06-01
Interaction of quantum radiation with multi-particle ensembles has sparked off intense research efforts during the past decade. Emblematic of this field is the quantum memory scheme, where a quantum state of light is mapped onto an ensemble of atoms and then recovered in its original shape. While opening new access to the basics of light-atom interaction, quantum memory also appears as a key element for information processing applications, such as linear optics quantum computation and long-distance quantum communication via quantum repeaters. Not surprisingly, it is far from trivial to practically recover a stored quantum state of light and, although impressive progress has already been accomplished, researchers are still struggling to reach this ambitious objective. This special issue provides an account of the state-of-the-art in a fast-moving research area that makes physicists, engineers and chemists work together at the forefront of their discipline, involving quantum fields and atoms in different media, magnetic resonance techniques and material science. Various strategies have been considered to store and retrieve quantum light. The explored designs belong to three main—while still overlapping—classes. In architectures derived from photon echo, information is mapped over the spectral components of inhomogeneously broadened absorption bands, such as those encountered in rare earth ion doped crystals and atomic gases in external gradient magnetic field. Protocols based on electromagnetic induced transparency also rely on resonant excitation and are ideally suited to the homogeneous absorption lines offered by laser cooled atomic clouds or ion Coulomb crystals. Finally off-resonance approaches are illustrated by Faraday and Raman processes. Coupling with an optical cavity may enhance the storage process, even for negligibly small atom number. Multiple scattering is also proposed as a way to enlarge the quantum interaction distance of light with matter. The
Hong, John; Hou, Bo; Lim, Jongchul; Pak, Sangyeon; Kim, Byung-Sung; Cho, Yuljae; Lee, Juwon; Lee, Young-Woo; Giraud, Paul; Lee, Sanghyo; Park, Jong Bae; Morris, Stephen M.; Snaith, Henry J.; Kim, Jong Min
2016-01-01
Colloidal quantum dots (CQDs) are extremely promising as photovoltaic materials. In particular, the tunability of their electronic band gap and cost effective synthetic procedures allow for the versatile fabrication of solar energy harvesting cells, resulting in optimal device performance. However, one of the main challenges in developing high performance quantum dot solar cells (QDSCs) is the improvement of the photo-generated charge transport and collection, which is mainly hindered by imperfect surface functionalization, such as the presence of surface electronic trap sites and the initial bulky surface ligands. Therefore, for these reasons, finding effective methods to efficiently decorate the surface of the as-prepared CQDs with new short molecular length chemical structures so as to enhance the performance of QDSCs is highly desirable. Here, we suggest employing hybrid halide ions along with the shortest heterocyclic molecule as a robust passivation structure to eliminate surface trap sites while decreasing the charge trapping dynamics and increasing the charge extraction efficiency in CQD active layers. This hybrid ligand treatment shows a better coordination with Pb atoms within the crystal, resulting in low trap sites and a near perfect removal of the pristine initial bulky ligands, thereby achieving better conductivity and film structure. Compared to halide ion-only treated cells, solar cells fabricated through this hybrid passivation method show an increase in the power conversion efficiency from 5.3% for the halide ion-treated cells to 6.8% for the hybrid-treated solar cells. PMID:29308200
Chang, Mou-Hsiung
2015-01-01
The classical probability theory initiated by Kolmogorov and its quantum counterpart, pioneered by von Neumann, were created at about the same time in the 1930s, but development of the quantum theory has trailed far behind. Although highly appealing, the quantum theory has a steep learning curve, requiring tools from both probability and analysis and a facility for combining the two viewpoints. This book is a systematic, self-contained account of the core of quantum probability and quantum stochastic processes for graduate students and researchers. The only assumed background is knowledge of the basic theory of Hilbert spaces, bounded linear operators, and classical Markov processes. From there, the book introduces additional tools from analysis, and then builds the quantum probability framework needed to support applications to quantum control and quantum information and communication. These include quantum noise, quantum stochastic calculus, stochastic quantum differential equations, quantum Markov semigrou...
Nonlinear optics quantum computing with circuit QED.
Adhikari, Prabin; Hafezi, Mohammad; Taylor, J M
2013-02-08
One approach to quantum information processing is to use photons as quantum bits and rely on linear optical elements for most operations. However, some optical nonlinearity is necessary to enable universal quantum computing. Here, we suggest a circuit-QED approach to nonlinear optics quantum computing in the microwave regime, including a deterministic two-photon phase gate. Our specific example uses a hybrid quantum system comprising a LC resonator coupled to a superconducting flux qubit to implement a nonlinear coupling. Compared to the self-Kerr nonlinearity, we find that our approach has improved tolerance to noise in the qubit while maintaining fast operation.
Scarani, Valerio
1998-01-01
The aim of this thesis was to explain what quantum computing is. The information for the thesis was gathered from books, scientific publications, and news articles. The analysis of the information revealed that quantum computing can be broken down to three areas: theories behind quantum computing explaining the structure of a quantum computer, known quantum algorithms, and the actual physical realizations of a quantum computer. The thesis reveals that moving from classical memor...
Wu, Lian-Ao; Lidar, Daniel A.
2005-01-01
When quantum communication networks proliferate they will likely be subject to a new type of attack: by hackers, virus makers, and other malicious intruders. Here we introduce the concept of "quantum malware" to describe such human-made intrusions. We offer a simple solution for storage of quantum information in a manner which protects quantum networks from quantum malware. This solution involves swapping the quantum information at random times between the network and isolated, distributed an...
Quantumness beyond quantum mechanics
International Nuclear Information System (INIS)
Sanz, Ángel S
2012-01-01
Bohmian mechanics allows us to understand quantum systems in the light of other quantum traits than the well-known ones (coherence, diffraction, interference, tunnelling, discreteness, entanglement, etc.). Here the discussion focusses precisely on two of these interesting aspects, which arise when quantum mechanics is thought within this theoretical framework: the non-crossing property, which allows for distinguishability without erasing interference patterns, and the possibility to define quantum probability tubes, along which the probability remains constant all the way. Furthermore, taking into account this hydrodynamic-like description as a link, it is also shown how this knowledge (concepts and ideas) can be straightforwardly transferred to other fields of physics (for example, the transmission of light along waveguides).
Nonlinear Dynamics In Quantum Physics -- Quantum Chaos and Quantum Instantons
Kröger, H.
2003-01-01
We discuss the recently proposed quantum action - its interpretation, its motivation, its mathematical properties and its use in physics: quantum mechanical tunneling, quantum instantons and quantum chaos.
Kearns, F L; Hudson, P S; Boresch, S; Woodcock, H L
2016-01-01
Enzyme activity is inherently linked to free energies of transition states, ligand binding, protonation/deprotonation, etc.; these free energies, and thus enzyme function, can be affected by residue mutations, allosterically induced conformational changes, and much more. Therefore, being able to predict free energies associated with enzymatic processes is critical to understanding and predicting their function. Free energy simulation (FES) has historically been a computational challenge as it requires both the accurate description of inter- and intramolecular interactions and adequate sampling of all relevant conformational degrees of freedom. The hybrid quantum mechanical molecular mechanical (QM/MM) framework is the current tool of choice when accurate computations of macromolecular systems are essential. Unfortunately, robust and efficient approaches that employ the high levels of computational theory needed to accurately describe many reactive processes (ie, ab initio, DFT), while also including explicit solvation effects and accounting for extensive conformational sampling are essentially nonexistent. In this chapter, we will give a brief overview of two recently developed methods that mitigate several major challenges associated with QM/MM FES: the QM non-Boltzmann Bennett's acceptance ratio method and the QM nonequilibrium work method. We will also describe usage of these methods to calculate free energies associated with (1) relative properties and (2) along reaction paths, using simple test cases with relevance to enzymes examples. © 2016 Elsevier Inc. All rights reserved.
Dynamics in the quantum/classical limit based on selective use of the quantum potential
International Nuclear Information System (INIS)
Garashchuk, Sophya; Dell’Angelo, David; Rassolov, Vitaly A.
2014-01-01
A classical limit of quantum dynamics can be defined by compensation of the quantum potential in the time-dependent Schrödinger equation. The quantum potential is a non-local quantity, defined in the trajectory-based form of the Schrödinger equation, due to Madelung, de Broglie, and Bohm, which formally generates the quantum-mechanical features in dynamics. Selective inclusion of the quantum potential for the degrees of freedom deemed “quantum,” defines a hybrid quantum/classical dynamics, appropriate for molecular systems comprised of light and heavy nuclei. The wavefunction is associated with all of the nuclei, and the Ehrenfest, or mean-field, averaging of the force acting on the classical degrees of freedom, typical of the mixed quantum/classical methods, is avoided. The hybrid approach is used to examine evolution of light/heavy systems in the harmonic and double-well potentials, using conventional grid-based and approximate quantum-trajectory time propagation. The approximate quantum force is defined on spatial domains, which removes unphysical coupling of the wavefunction fragments corresponding to distinct classical channels or configurations. The quantum potential, associated with the quantum particle, generates forces acting on both quantum and classical particles to describe the backreaction
Dynamics in the quantum/classical limit based on selective use of the quantum potential
Energy Technology Data Exchange (ETDEWEB)
Garashchuk, Sophya, E-mail: garashchuk@sc.edu; Dell’Angelo, David; Rassolov, Vitaly A. [Department of Chemistry and Biochemistry, University of South Carolina, Columbia, South Carolina 29208 (United States)
2014-12-21
A classical limit of quantum dynamics can be defined by compensation of the quantum potential in the time-dependent Schrödinger equation. The quantum potential is a non-local quantity, defined in the trajectory-based form of the Schrödinger equation, due to Madelung, de Broglie, and Bohm, which formally generates the quantum-mechanical features in dynamics. Selective inclusion of the quantum potential for the degrees of freedom deemed “quantum,” defines a hybrid quantum/classical dynamics, appropriate for molecular systems comprised of light and heavy nuclei. The wavefunction is associated with all of the nuclei, and the Ehrenfest, or mean-field, averaging of the force acting on the classical degrees of freedom, typical of the mixed quantum/classical methods, is avoided. The hybrid approach is used to examine evolution of light/heavy systems in the harmonic and double-well potentials, using conventional grid-based and approximate quantum-trajectory time propagation. The approximate quantum force is defined on spatial domains, which removes unphysical coupling of the wavefunction fragments corresponding to distinct classical channels or configurations. The quantum potential, associated with the quantum particle, generates forces acting on both quantum and classical particles to describe the backreaction.
Wang, Lei; Tricard, Simon; Yue, Pengwei; Zhao, Jihua; Fang, Jian; Shen, Weiguo
2016-03-15
A novel polypyrrole (PPy) and graphene quantum dots (GQDs) @ Prussian Blue (PB) nanocomposite has been grafted on a graphite felt (GF) substrate (PPy/GQDs@PB/GF), and has been proven to be an efficient electrochemical sensor for the determination of l-cysteine (l-cys). GQDs, which were fabricated by carbonization of citric acid and adsorbed on GF surface ultrasonically, played an important role for promoting the synthesis process of PB via a spontaneous redox reaction between Fe(3+) and [Fe(CN)6](3-). The PPy film has been electro-polymerized to improve the electrochemical stability of the PPy/GQDs@PB/GF electrode. The as-prepared electrode was characterized by scanning electron microscopy (SEM), transmission electron microscopy (TEM), infrared spectroscopy (IR), X-ray diffraction (XRD) and electrochemical methods. It exhibited an excellent activity for the electrocatalytic oxidation of l-cys, with a detection sensitivity equal to 0.41 Amol(-1) L for a concentration range of 0.2-50 μmolL(-1), and equal to 0.15 Amol(-1) L for a concentration range of 50-1000 μmolL(-1). A low detection limit of 0.15 μmolL(-1), as well as a remarkable long-time stability and a negligible sensitivity to interfering analytes, were also ascertained. Copyright © 2015 Elsevier B.V. All rights reserved.
Kovalev, Vadim M; Tse, Wang-Kong
2017-11-22
We develop a microscopic theory for the relaxation dynamics of an optically pumped two-level system (TLS) coupled to a bath of weakly interacting Bose gas. Using Keldysh formalism and diagrammatic perturbation theory, expressions for the relaxation times of the TLS Rabi oscillations are derived when the boson bath is in the normal state and the Bose-Einstein condensate (BEC) state. We apply our general theory to consider an irradiated quantum dot coupled with a boson bath consisting of a two-dimensional dipolar exciton gas. When the bath is in the BEC regime, relaxation of the Rabi oscillations is due to both condensate and non-condensate fractions of the bath bosons for weak TLS-light coupling and pre dominantly due to the non-condensate fraction for strong TLS-light coupling. Our theory also shows that a phase transition of the bath from the normal to the BEC state strongly influences the relaxation rate of the TLS Rabi oscillations. The TLS relaxation rate is approximately independent of the pump field frequency and monotonically dependent on the field strength when the bath is in the low-temperature regime of the normal phase. Phase transition of the dipolar exciton gas leads to a non-monotonic dependence of the TLS relaxation rate on both the pump field frequency and field strength, providing a characteristic signature for the detection of BEC phase transition of the coupled dipolar exciton gas.
Woo Choi, Jin; Woo, Hee Chul; Huang, Xiaoguang; Jung, Wan-Gil; Kim, Bong-Joong; Jeon, Sie-Wook; Yim, Sang-Youp; Lee, Jae-Suk; Lee, Chang-Lyoul
2018-05-22
The photoluminescence quantum yield (PLQY) and charge carrier mobility of organic-inorganic perovskite QDs were enhanced by the optimization of crystallinity and surface passivation as well as solid-state ligand exchange. The crystallinity of perovskite QDs was determined by the Effective solvent field (Esol) of various solvents for precipitation. The solvent with high Esol could more quickly countervail the localized field generated by the polar solvent, and it causes fast crystallization of the dissolved precursor, which results in poor crystallinity. The post-ligand adding process (PLAP) and post-ligand exchange process (PLEP) increase the PLQY of perovskite QDs by reducing non-radiative recombination and the density of surface defect states through surface passivation. Particularly, the post ligand exchange process (PLEP) in the solid-state improved the charge carrier mobility of perovskite QDs in addition to the PLQY enhancement. The ligand exchange with short alkyl chain length ligands could improve the packing density of perovskite QDs in films by reducing the inter-particle distance between perovskite QDs. The maximum hole mobility of 6.2 × 10-3 cm2 V-1 s-1, one order higher than that of pristine QDs without the PLEP, is obtained at perovskite QDs with hexyl ligands. By using PLEP treatment, compared to the pristine device, a 2.5 times higher current efficiency in perovskite QD-LEDs was achieved due to the improved charge carrier mobility and PLQY.
Classical Limit and Quantum Logic
Losada, Marcelo; Fortin, Sebastian; Holik, Federico
2018-02-01
The analysis of the classical limit of quantum mechanics usually focuses on the state of the system. The general idea is to explain the disappearance of the interference terms of quantum states appealing to the decoherence process induced by the environment. However, in these approaches it is not explained how the structure of quantum properties becomes classical. In this paper, we consider the classical limit from a different perspective. We consider the set of properties of a quantum system and we study the quantum-to-classical transition of its logical structure. The aim is to open the door to a new study based on dynamical logics, that is, logics that change over time. In particular, we appeal to the notion of hybrid logics to describe semiclassical systems. Moreover, we consider systems with many characteristic decoherence times, whose sublattices of properties become distributive at different times.
Quantum photonics with quantum dots in photonic wires
DEFF Research Database (Denmark)
Munsch, Mathieu; Kuhlmann, Andreas; Cadeddu, Davide
2016-01-01
We present results from the spectroscopy of a single quantum dot in a photonic wire. The device presents a high photon extraction efficiency, and strong hybrid coupling to mechanical modes. We use resonance fluorescence to probe the emitter’s properties with the highest sensitivity. Weperform...
Quantum optics with quantum dots in photonic wires
DEFF Research Database (Denmark)
Munsch, Mathieu; Cadeddu, Davide; Teissier, Jean
2016-01-01
We present an exploration of the spectroscopy of a single quantum dot in a photonic wire. The device presents a high photon extraction efficiency, and strong hybrid coupling to mechanical modes. We use resonance fluorescence to probe the emitter's properties with the highest sensitivity, allowing...
International Nuclear Information System (INIS)
Anon.
1990-01-01
The book is on quantum mechanics. The emphasis is on the basic concepts and the methodology. The chapters include: Breakdown of classical concepts; Quantum mechanical concepts; Basic postulates of quantum mechanics; solution of problems in quantum mechanics; Simple harmonic oscillator; and Angular Momentum
International Nuclear Information System (INIS)
Buechler, Hans Peter; Calcarco, Tommaso; Dressel, Martin
2008-01-01
The following topics are dealt with: Artificial atoms and molecules, tailored from solids, fractional flux quanta, molecular magnets, controlled interaction in quantum gases, the theory of quantum correlations in mott matter, cold gases, and mesoscopic systems, Bose-Einstein condensates on the chip, on the route to the quantum computer, a quantum computer in diamond. (HSI)
International Nuclear Information System (INIS)
Reynaud, S.; Giacobino, S.; Zinn-Justin, J.
1997-01-01
This course is dedicated to present in a pedagogical manner the recent developments in peculiar fields concerned by quantum fluctuations: quantum noise in optics, light propagation through dielectric media, sub-Poissonian light generated by lasers and masers, quantum non-demolition measurements, quantum electrodynamics applied to cavities and electrical circuits involving superconducting tunnel junctions. (A.C.)
Jabeen, Uzma; Adhikari, Tham; Pathak, Dinesh; Shah, Syed Mujtaba; Nunzi, Jean-Michel
2018-04-01
Cadmium sulphide (CdS) and Mn-doped CdS nanocrystals were synthesized by co-precipitation method. The nanocrystals were characterized by Fluorescence, Fourier Transformed Infra-red Spectrometer (FTIR), UV-Visible, X-ray diffraction (XRD), X-ray photoelectron spectrometer (XPS), Field Emission Scanning Electron Microscope (FESEM), and High Resolution Transmission Electron Microscope (HRTEM). A considerable blue shift of absorption band with respect to the cadmium sulphide was observed by the Mn concentration (0.5 M) in the doped sample with decreasing the size of nanocrystals. Other reason for this may be Mn doping. Subsequently the band gap was altered from 2.11 to 2.21 eV due to quantum confinement effect. Scanning electron microscope supplemented with EDAX was operated to find grain size and chemical composition of the synthesized nanomaterials. The PL spectrum of Mn-doped CdS nanocrystals displays three PL bands the first one, within the range of 500 nm and the second band at 537 nm, and the third one around 713 nm is labelled red band emission due to attributed to a 4T1→6A1 transition within the 3d shell of divalent manganese. XRD analysis showed that the material was in cubic crystalline state. A comparative study of surfaces of un-doped and metal doped CdS nanocrystals were investigated using X-ray Photoelectron Spectroscopy (XPS). The synthesized nanomaterial in combination with polymer, poly (3-hexyl thiophene) was operated in the construction of photovoltaic cells. The photovoltaic devices with CdS nanocrystals exhibited power conversion efficiency of 0.34% without annealing and 0.38% with annealing. However, the power conversion efficiency was enhanced by a factor of 0.35 without annealing and 0.42 with annealing with corporation of Mn impurity in CdS lattice. Atomic Force Microscopy was employed for morphology and packing behavior of blend of nanocrystals with organic polymer.
Lanzagorta, Marco
2011-01-01
This book offers a concise review of quantum radar theory. Our approach is pedagogical, making emphasis on the physics behind the operation of a hypothetical quantum radar. We concentrate our discussion on the two major models proposed to date: interferometric quantum radar and quantum illumination. In addition, this book offers some new results, including an analytical study of quantum interferometry in the X-band radar region with a variety of atmospheric conditions, a derivation of a quantum radar equation, and a discussion of quantum radar jamming.This book assumes the reader is familiar w
Glueballs, hybrids, multiquarks
Energy Technology Data Exchange (ETDEWEB)
Klempt, Eberhard [Helmholtz-Institut fuer Strahlen-und Kernphysik der Rheinischen Friedrich-Wilhelms Universitaet, Nussallee 14-16, D-53115 Bonn (Germany)], E-mail: klempt@hiskp.uni-bonn.de; Zaitsev, Alexander [Institute for High-Energy Physics, Moscow Region, RU-142284 Protvino (Russian Federation)
2007-12-15
Glueballs, hybrids and multiquark states are predicted as bound states in models guided by quantum chromo dynamics (QCD), by QCD sum rules or QCD on a lattice. Estimates for the (scalar) glueball ground state are in the mass range from 1000 to 1800 MeV, followed by a tensor and a pseudoscalar glueball at higher mass. Experiments have reported evidence for an abundance of meson resonances with 0{sup -+},0{sup ++} and 2{sup ++} quantum numbers. In particular, the sector of scalar mesons is full of surprises starting from the elusive {sigma} and {kappa} mesons. The a{sub 0}(980) and f{sub 0}(980), discussed extensively in the literature, are reviewed with emphasis on their Janus-like appearance as KK-bar molecules, tetraquark states or qq-bar mesons. Most exciting is the possibility that the three mesons f{sub 0}(1370), f{sub 0}(1500), and f{sub 0}(1710) might reflect the appearance of a scalar glueball in the world of quarkonia. However, the existence of f{sub 0}(1370) is not beyond doubt and there is evidence that both f{sub 0}(1500) and f{sub 0}(1710) are flavour octet states, possibly in a tetraquark composition. We suggest a scheme in which the scalar glueball is dissolved into the wide background into which all scalar flavour-singlet mesons collapse. There is an abundance of meson resonances with the quantum numbers of the {eta}. Three states are reported below 1.5GeV/c{sup 2} whereas quark models expect only one, perhaps two. One of these states, {iota}(1440), was the prime glueball candidate for a long time. We show that {iota}(1440) is the first radial excitation of the {eta} meson. Hybrids may have exotic quantum numbers which are not accessible by qq-bar mesons. There are several claims for J{sup PC}=1{sup -+} exotics, some of them with properties as predicted from the flux tube model interpreting the quark-antiquark binding by a gluon string. The evidence for these states depends partly on the assumption that meson-meson interactions are dominated by s
Quantum acoustics with superconducting qubits
Chu, Yiwen
2017-04-01
The ability to engineer and manipulate different types of quantum mechanical objects allows us to take advantage of their unique properties and create useful hybrid technologies. Thus far, complex quantum states and exquisite quantum control have been demonstrated in systems ranging from trapped ions to superconducting resonators. Recently, there have been many efforts to extend these demonstrations to the motion of complex, macroscopic objects. These mechanical objects have important applications as quantum memories or transducers for measuring and connecting different types of quantum systems. In particular, there have been a few experiments that couple motion to nonlinear quantum objects such as superconducting qubits. This opens up the possibility of creating, storing, and manipulating non-Gaussian quantum states in mechanical degrees of freedom. However, before sophisticated quantum control of mechanical motion can be achieved, we must realize systems with long coherence times while maintaining a sufficient interaction strength. These systems should be implemented in a simple and robust manner that allows for increasing complexity and scalability in the future. In this talk, I will describe our recent experiments demonstrating a high frequency bulk acoustic wave resonator that is strongly coupled to a superconducting qubit using piezoelectric transduction. In contrast to previous experiments with qubit-mechanical systems, our device requires only simple fabrication methods, extends coherence times to many microseconds, and provides controllable access to a multitude of phonon modes. We use this system to demonstrate basic quantum operations on the coupled qubit-phonon system. Straightforward improvements to the current device will allow for advanced protocols analogous to what has been shown in optical and microwave resonators, resulting in a novel resource for implementing hybrid quantum technologies.
Quantum phase transitions in semilocal quantum liquids
Iqbal, Nabil; Liu, Hong; Mezei, Márk
2015-01-01
We consider several types of quantum critical phenomena from finite-density gauge-gravity duality which to different degrees lie outside the Landau-Ginsburg-Wilson paradigm. These include: (i) a "bifurcating" critical point, for which the order parameter remains gapped at the critical point, and thus is not driven by soft order parameter fluctuations. Rather it appears to be driven by "confinement" which arises when two fixed points annihilate and lose conformality. On the condensed side, there is an infinite tower of condensed states and the nonlinear response of the tower exhibits an infinite spiral structure; (ii) a "hybridized" critical point which can be described by a standard Landau-Ginsburg sector of order parameter fluctuations hybridized with a strongly coupled sector; (iii) a "marginal" critical point which is obtained by tuning the above two critical points to occur together and whose bosonic fluctuation spectrum coincides with that postulated to underly the "Marginal Fermi Liquid" description of the optimally doped cuprates.
International Nuclear Information System (INIS)
Kilin, Sergei Ya
1999-01-01
A new research direction known as quantum information is a multidisciplinary subject which involves quantum mechanics, optics, information theory, programming, discrete mathematics, laser physics and spectroscopy, and depends heavily on contributions from such areas as quantum computing, quantum teleportation and quantum cryptography, decoherence studies, and single-molecule and impurity spectroscopy. Some new results achieved in this rapidly growing field are discussed. (reviews of topical problems)
Energy Technology Data Exchange (ETDEWEB)
Kilin, Sergei Ya [B.I. Stepanov Institute of Physics, National Academy of Sciences of Belarus, Minsk (Belarus)
1999-05-31
A new research direction known as quantum information is a multidisciplinary subject which involves quantum mechanics, optics, information theory, programming, discrete mathematics, laser physics and spectroscopy, and depends heavily on contributions from such areas as quantum computing, quantum teleportation and quantum cryptography, decoherence studies, and single-molecule and impurity spectroscopy. Some new results achieved in this rapidly growing field are discussed. (reviews of topical problems)
International Nuclear Information System (INIS)
Stapp, H.P.
1988-12-01
Quantum ontologies are conceptions of the constitution of the universe that are compatible with quantum theory. The ontological orientation is contrasted to the pragmatic orientation of science, and reasons are given for considering quantum ontologies both within science, and in broader contexts. The principal quantum ontologies are described and evaluated. Invited paper at conference: Bell's Theorem, Quantum Theory, and Conceptions of the Universe, George Mason University, October 20-21, 1988. 16 refs
Quantum Computer Games: Quantum Minesweeper
Gordon, Michal; Gordon, Goren
2010-01-01
The computer game of quantum minesweeper is introduced as a quantum extension of the well-known classical minesweeper. Its main objective is to teach the unique concepts of quantum mechanics in a fun way. Quantum minesweeper demonstrates the effects of superposition, entanglement and their non-local characteristics. While in the classical…
Entanglement and quantum superposition induced by a single photon
Lü, Xin-You; Zhu, Gui-Lei; Zheng, Li-Li; Wu, Ying
2018-03-01
We predict the occurrence of single-photon-induced entanglement and quantum superposition in a hybrid quantum model, introducing an optomechanical coupling into the Rabi model. Originally, it comes from the photon-dependent quantum property of the ground state featured by the proposed hybrid model. It is associated with a single-photon-induced quantum phase transition, and is immune to the A2 term of the spin-field interaction. Moreover, the obtained quantum superposition state is actually a squeezed cat state, which can significantly enhance precision in quantum metrology. This work offers an approach to manipulate entanglement and quantum superposition with a single photon, which might have potential applications in the engineering of new single-photon quantum devices, and also fundamentally broaden the regime of cavity QED.
Combined quantum and molecular mechanics (QM/MM).
Friesner, Richard A
2004-12-01
We describe the current state of the art of mixed quantum mechanics/molecular mechanics (QM/MM) methodology, with a particular focus on modeling of enzymatic reactions. Over the past decade, the effectiveness of these methods has increased dramatically, based on improved quantum chemical methods, advances in the description of the QM/MM interface, and reductions in the cost/performance of computing hardware. Two examples of pharmaceutically relevant applications, cytochrome P450 and class C β-lactamase, are presented.: © 2004 Elsevier Ltd . All rights reserved.
A repeat-until-success quantum computing scheme
Energy Technology Data Exchange (ETDEWEB)
Beige, A [School of Physics and Astronomy, University of Leeds, Leeds LS2 9JT (United Kingdom); Lim, Y L [DSO National Laboratories, 20 Science Park Drive, Singapore 118230, Singapore (Singapore); Kwek, L C [Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117542, Singapore (Singapore)
2007-06-15
Recently we proposed a hybrid architecture for quantum computing based on stationary and flying qubits: the repeat-until-success (RUS) quantum computing scheme. The scheme is largely implementation independent. Despite the incompleteness theorem for optical Bell-state measurements in any linear optics set-up, it allows for the implementation of a deterministic entangling gate between distant qubits. Here we review this distributed quantum computation scheme, which is ideally suited for integrated quantum computation and communication purposes.
A repeat-until-success quantum computing scheme
International Nuclear Information System (INIS)
Beige, A; Lim, Y L; Kwek, L C
2007-01-01
Recently we proposed a hybrid architecture for quantum computing based on stationary and flying qubits: the repeat-until-success (RUS) quantum computing scheme. The scheme is largely implementation independent. Despite the incompleteness theorem for optical Bell-state measurements in any linear optics set-up, it allows for the implementation of a deterministic entangling gate between distant qubits. Here we review this distributed quantum computation scheme, which is ideally suited for integrated quantum computation and communication purposes
Traffic Flow Optimization Using a Quantum Annealer
Directory of Open Access Journals (Sweden)
Florian Neukart
2017-12-01
Full Text Available Quantum annealing algorithms belong to the class of metaheuristic tools, applicable for solving binary optimization problems. Hardware implementations of quantum annealing, such as the quantum processing units (QPUs produced by D-Wave Systems, have been subject to multiple analyses in research, with the aim of characterizing the technology’s usefulness for optimization and sampling tasks. In this paper, we present a real-world application that uses quantum technologies. Specifically, we show how to map certain parts of a real-world traffic flow optimization problem to be suitable for quantum annealing. We show that time-critical optimization tasks, such as continuous redistribution of position data for cars in dense road networks, are suitable candidates for quantum computing. Due to the limited size and connectivity of current-generation D-Wave QPUs, we use a hybrid quantum and classical approach to solve the traffic flow problem.
Energy Technology Data Exchange (ETDEWEB)
Drummond, P D [University of Queensland, St. Lucia, QLD (Australia).Physics Department
1999-07-01
Full text: Quantum optics in Australia has been an active research field for some years. I shall focus on recent developments in quantum and atom optics. Generally, the field as a whole is becoming more and more diverse, as technological developments drive experiments into new areas, and theorists either attempt to explain the new features, or else develop models for even more exotic ideas. The recent developments include quantum solitons, quantum computing, Bose-Einstein condensation, atom lasers, quantum cryptography, and novel tests of quantum mechanics. The talk will briefly cover current progress and outstanding problems in each of these areas. Copyright (1999) Australian Optical Society.
Quantum entanglement and quantum teleportation
International Nuclear Information System (INIS)
Shih, Y.H.
2001-01-01
One of the most surprising consequences of quantum mechanics is the entanglement of two or more distance particles. The ''ghost'' interference and the ''ghost'' image experiments demonstrated the astonishing nonlocal behavior of an entangled photon pair. Even though we still have questions in regard to fundamental issues of the entangled quantum systems, quantum entanglement has started to play important roles in quantum information and quantum computation. Quantum teleportation is one of the hot topics. We have demonstrated a quantum teleportation experiment recently. The experimental results proved the working principle of irreversibly teleporting an unknown arbitrary quantum state from one system to another distant system by disassembling into and then later reconstructing from purely classical information and nonclassical EPR correlations. The distinct feature of this experiment is that the complete set of Bell states can be distinguished in the Bell state measurement. Teleportation of a quantum state can thus occur with certainty in principle. (orig.)
Czech Academy of Sciences Publication Activity Database
Sklenák, Štěpán; Dědeček, Jiří; Li, Chengbin; Wichterlová, Blanka; Gábová, Vendula; Sierka, M.; Sauer, J.
2007-01-01
Roč. 46, č. 38 (2007), s. 7286-7289 ISSN 1433-7851 R&D Projects: GA AV ČR 1ET400400413; GA ČR GA203/06/1449; GA AV ČR IAA4040308 Institutional research plan: CEZ:AV0Z40400503 Keywords : MQ MAS NMR * chemical-shifts * ab-initio * catalysts Subject RIV: CF - Physical ; Theoretical Chemistry Impact factor: 10.031, year: 2007
Ridder, L.; Rietjens, I.M.C.M.; Vervoort, J.J.M.; Mulholland, A.J.
2002-01-01
Glutathione S-transferases (GSTs) play an important role in the detoxification of xenobiotics in mammals. They catalyze the conjugation of glutathione to a wide range of electrophilic compounds. Phenanthrene 9,10-oxide is a model substrate for GSTs, representing an important group of epoxide
Zeng, Xiancheng; Hu, Xiangqian; Yang, Weitao
2012-12-11
A fragment-based fractional number of electron (FNE) approach, is developed to study entire electron transfer (ET) processes from the electron donor region to the acceptor region in condensed phase. Both regions are described by the density-fragment interaction (DFI) method while FNE as an efficient ET order parameter is applied to simulate the electron transfer process. In association with the QM/MM energy expression, the DFI-FNE method is demonstrated to describe ET processes robustly with the Ru 2+ -Ru 3+ self-exchange ET as a proof-of-concept example. This method allows for systematic calculations of redox free energies, reorganization energies, and electronic couplings, and the absolute ET rate constants within the Marcus regime.
Quantum robots and quantum computers
Energy Technology Data Exchange (ETDEWEB)
Benioff, P.
1998-07-01
Validation of a presumably universal theory, such as quantum mechanics, requires a quantum mechanical description of systems that carry out theoretical calculations and systems that carry out experiments. The description of quantum computers is under active development. No description of systems to carry out experiments has been given. A small step in this direction is taken here by giving a description of quantum robots as mobile systems with on board quantum computers that interact with different environments. Some properties of these systems are discussed. A specific model based on the literature descriptions of quantum Turing machines is presented.
Quantum computers and quantum computations
International Nuclear Information System (INIS)
Valiev, Kamil' A
2005-01-01
This review outlines the principles of operation of quantum computers and their elements. The theory of ideal computers that do not interact with the environment and are immune to quantum decohering processes is presented. Decohering processes in quantum computers are investigated. The review considers methods for correcting quantum computing errors arising from the decoherence of the state of the quantum computer, as well as possible methods for the suppression of the decohering processes. A brief enumeration of proposed quantum computer realizations concludes the review. (reviews of topical problems)
Chanda, Rajat
1997-01-01
The book discusses the laws of quantum mechanics, several amazing quantum phenomena and some recent progress in understanding the connection between the quantum and the classical worlds. We show how paradoxes arise and how to resolve them. The significance of Bell's theorem and the remarkable experimental results on particle correlations are described in some detail. Finally, the current status of our understanding of quantum theory is summerised.
Stochastic effects in hybrid inflation
Martin, Jérôme; Vennin, Vincent
2012-02-01
Hybrid inflation is a two-field model where inflation ends due to an instability. In the neighborhood of the instability point, the potential is very flat and the quantum fluctuations dominate over the classical motion of the inflaton and waterfall fields. In this article, we study this regime in the framework of stochastic inflation. We numerically solve the two coupled Langevin equations controlling the evolution of the fields and compute the probability distributions of the total number of e-folds and of the inflation exit point. Then, we discuss the physical consequences of our results, in particular, the question of how the quantum diffusion can affect the observable predictions of hybrid inflation.
Coleman, Piers; Schofield, Andrew J
2005-01-20
As we mark the centenary of Albert Einstein's seminal contribution to both quantum mechanics and special relativity, we approach another anniversary--that of Einstein's foundation of the quantum theory of solids. But 100 years on, the same experimental measurement that puzzled Einstein and his contemporaries is forcing us to question our understanding of how quantum matter transforms at ultra-low temperatures.
Indian Academy of Sciences (India)
In the first part of this article, we had looked at how quantum physics can be harnessed to make the building blocks of a quantum computer. In this concluding part, we look at algorithms which can exploit the power of this computational device, and some practical difficulties in building such a device. Quantum Algorithms.
I, Quantum Robot: Quantum Mind control on a Quantum Computer
Zizzi, Paola
2008-01-01
The logic which describes quantum robots is not orthodox quantum logic, but a deductive calculus which reproduces the quantum tasks (computational processes, and actions) taking into account quantum superposition and quantum entanglement. A way toward the realization of intelligent quantum robots is to adopt a quantum metalanguage to control quantum robots. A physical implementation of a quantum metalanguage might be the use of coherent states in brain signals.
International Nuclear Information System (INIS)
Moir, R.W.
1980-01-01
The rationale for hybrid fusion-fission reactors is the production of fissile fuel for fission reactors. A new class of reactor, the fission-suppressed hybrid promises unusually good safety features as well as the ability to support 25 light-water reactors of the same nuclear power rating, or even more high-conversion-ratio reactors such as the heavy-water type. One 4000-MW nuclear hybrid can produce 7200 kg of 233 U per year. To obtain good economics, injector efficiency times plasma gain (eta/sub i/Q) should be greater than 2, the wall load should be greater than 1 MW.m -2 , and the hybrid should cost less than 6 times the cost of a light-water reactor. Introduction rates for the fission-suppressed hybrid are usually rapid
Protein Structure Validation and Refinement Using Chemical Shifts Derived from Quantum Mechanics
DEFF Research Database (Denmark)
Bratholm, Lars Andersen
to within 3 A. Furthermore, a fast quantum mechanics based chemical shift predictor was developed together with methodology for using chemical shifts in structure simulations. The developed predictor was used for renement of several protein structures and for reducing the computational cost of quantum...... mechanics / molecular mechanics (QM/MM) computations of chemical shieldings. Several improvements to the predictor is ongoing, where among other things, kernel based machine learning techniques have successfully been used to improve the quantum mechanical level of theory used in the predictions....
Quantum Logic and Quantum Reconstruction
Stairs, Allen
2015-01-01
Quantum logic understood as a reconstruction program had real successes and genuine limitations. This paper offers a synopsis of both and suggests a way of seeing quantum logic in a larger, still thriving context.
Quantum dynamics of quantum bits
International Nuclear Information System (INIS)
Nguyen, Bich Ha
2011-01-01
The theory of coherent oscillations of the matrix elements of the density matrix of the two-state system as a quantum bit is presented. Different calculation methods are elaborated in the case of a free quantum bit. Then the most appropriate methods are applied to the study of the density matrices of the quantum bits interacting with a classical pumping radiation field as well as with the quantum electromagnetic field in a single-mode microcavity. The theory of decoherence of a quantum bit in Markovian approximation is presented. The decoherence of a quantum bit interacting with monoenergetic photons in a microcavity is also discussed. The content of the present work can be considered as an introduction to the study of the quantum dynamics of quantum bits. (review)
Quantum logic between remote quantum registers
Yao, N. Y.; Gong, Z.-X.; Laumann, C. R.; Bennett, S. D.; Duan, L.-M.; Lukin, M. D.; Jiang, L.; Gorshkov, A. V.
2013-02-01
We consider two approaches to dark-spin-mediated quantum computing in hybrid solid-state spin architectures. First, we review the notion of eigenmode-mediated unpolarized spin-chain state transfer and extend the analysis to various experimentally relevant imperfections: quenched disorder, dynamical decoherence, and uncompensated long-range coupling. In finite-length chains, the interplay between disorder-induced localization and decoherence yields a natural optimal channel fidelity, which we calculate. Long-range dipolar couplings induce a finite intrinsic lifetime for the mediating eigenmode; extensive numerical simulations of dipolar chains of lengths up to L=12 show remarkably high fidelity despite these decay processes. We further briefly consider the extension of the protocol to bosonic systems of coupled oscillators. Second, we introduce a quantum mirror based architecture for universal quantum computing that exploits all of the dark spins in the system as potential qubits. While this dramatically increases the number of qubits available, the composite operations required to manipulate dark-spin qubits significantly raise the error threshold for robust operation. Finally, we demonstrate that eigenmode-mediated state transfer can enable robust long-range logic between spatially separated nitrogen-vacancy registers in diamond; disorder-averaged numerics confirm that high-fidelity gates are achievable even in the presence of moderate disorder.
Brown, Matthew J.
2014-02-01
The framework of quantum frames can help unravel some of the interpretive difficulties i the foundation of quantum mechanics. In this paper, I begin by tracing the origins of this concept in Bohr's discussion of quantum theory and his theory of complementarity. Engaging with various interpreters and followers of Bohr, I argue that the correct account of quantum frames must be extended beyond literal space-time reference frames to frames defined by relations between a quantum system and the exosystem or external physical frame, of which measurement contexts are a particularly important example. This approach provides superior solutions to key EPR-type measurement and locality paradoxes.
Zurek, Wojciech Hubert
2009-03-01
Quantum Darwinism describes the proliferation, in the environment, of multiple records of selected states of a quantum system. It explains how the quantum fragility of a state of a single quantum system can lead to the classical robustness of states in their correlated multitude; shows how effective `wave-packet collapse' arises as a result of the proliferation throughout the environment of imprints of the state of the system; and provides a framework for the derivation of Born's rule, which relates the probabilities of detecting states to their amplitudes. Taken together, these three advances mark considerable progress towards settling the quantum measurement problem.
International Nuclear Information System (INIS)
Kouwenhoven, L.; Marcus, C.
1998-01-01
Quantum dots are man-made ''droplets'' of charge that can contain anything from a single electron to a collection of several thousand. Their typical dimensions range from nanometres to a few microns, and their size, shape and interactions can be precisely controlled through the use of advanced nanofabrication technology. The physics of quantum dots shows many parallels with the behaviour of naturally occurring quantum systems in atomic and nuclear physics. Indeed, quantum dots exemplify an important trend in condensed-matter physics in which researchers study man-made objects rather than real atoms or nuclei. As in an atom, the energy levels in a quantum dot become quantized due to the confinement of electrons. With quantum dots, however, an experimentalist can scan through the entire periodic table by simply changing a voltage. In this article the authors describe how quantum dots make it possible to explore new physics in regimes that cannot otherwise be accessed in the laboratory. (UK)
Quantum information. Teleporation - cryptography - quantum computer
International Nuclear Information System (INIS)
Breuer, Reinhard
2010-01-01
The following topics are dealt with: Reality in the test house, quantum teleportation, 100 years of quantum theory, the reality of quanta, interactionless quantum measurement, rules for quantum computers, quantum computers with ions, spintronics with diamond, the limits of the quantum computers, a view into the future of quantum optics. (HSI)
Quantum symmetry in quantum theory
International Nuclear Information System (INIS)
Schomerus, V.
1993-02-01
Symmetry concepts have always been of great importance for physical problems like explicit calculations, classification or model building. More recently, new 'quantum symmetries' ((quasi) quantum groups) attracted much interest in quantum theory. It is shown that all these quantum symmetries permit a conventional formulation as symmetry in quantum mechanics. Symmetry transformations can act on the Hilbert space H of physical states such that the ground state is invariant and field operators transform covariantly. Models show that one must allow for 'truncation' in the tensor product of representations of a quantum symmetry. This means that the dimension of the tensor product of two representations of dimension σ 1 and σ 2 may be strictly smaller than σ 1 σ 2 . Consistency of the transformation law of field operators local braid relations leads us to expect, that (weak) quasi quantum groups are the most general symmetries in local quantum theory. The elements of the R-matrix which appears in these local braid relations turn out to be operators on H in general. It will be explained in detail how examples of field algebras with weak quasi quantum group symmetry can be obtained. Given a set of observable field with a finite number of superselection sectors, a quantum symmetry together with a complete set of covariant field operators which obey local braid relations are constructed. A covariant transformation law for adjoint fields is not automatic but will follow when the existence of an appropriate antipode is assumed. At the example of the chiral critical Ising model, non-uniqueness of the quantum symmetry will be demonstrated. Generalized quantum symmetries yield examples of gauge symmetries in non-commutative geometry. Quasi-quantum planes are introduced as the simplest examples of quasi-associative differential geometry. (Weak) quasi quantum groups can act on them by generalized derivations much as quantum groups do in non-commutative (differential-) geometry
Quantum geometry in dynamical Regge calculus
International Nuclear Information System (INIS)
Hagura, Hiroyuki
2002-01-01
We study geometric properties of dynamical Regge calculus which is a hybridization of dynamical triangulation and quantum Regge calculus. Lattice diffeomorphisms are generated by certain elementary moves on a simplicial lattice in the hybrid model. At the semiclassical level, we discuss a possibility that the lattice diffeomorphisms give a simple explanation for the Bekenstein-Hawking entropy of a black hole. At the quantum level, numerical calculations of 3D pure gravity show that a fractal structure of the hybrid model is the same as that of dynamical triangulation in the strong-coupling phase. In the weak-coupling phase, on the other hand, space-time becomes a spiky configuration, which often occurs in quantum Regge calculus
CSIR Research Space (South Africa)
Jacob John, Maya
2009-04-01
Full Text Available mixed short sisal/glass hybrid fibre reinforced low density polyethylene composites was investigated by Kalaprasad et al [25].Chemical surface modifications such as alkali, acetic anhydride, stearic acid, permanganate, maleic anhydride, silane...
Cetorelli, Nicola
2014-01-01
I introduce the concept of hybrid intermediaries: financial conglomerates that control a multiplicity of entity types active in the "assembly line" process of modern financial intermediation, a system that has become known as shadow banking. The complex bank holding companies of today are the best example of hybrid intermediaries, but I argue that financial firms from the "nonbank" space can just as easily evolve into conglomerates with similar organizational structure, thus acquiring the cap...
Quantum games as quantum types
Delbecque, Yannick
In this thesis, we present a new model for higher-order quantum programming languages. The proposed model is an adaptation of the probabilistic game semantics developed by Danos and Harmer [DH02]: we expand it with quantum strategies which enable one to represent quantum states and quantum operations. Some of the basic properties of these strategies are established and then used to construct denotational semantics for three quantum programming languages. The first of these languages is a formalisation of the measurement calculus proposed by Danos et al. [DKP07]. The other two are new: they are higher-order quantum programming languages. Previous attempts to define a denotational semantics for higher-order quantum programming languages have failed. We identify some of the key reasons for this and base the design of our higher-order languages on these observations. The game semantics proposed in this thesis is the first denotational semantics for a lambda-calculus equipped with quantum types and with extra operations which allow one to program quantum algorithms. The results presented validate the two different approaches used in the design of these two new higher-order languages: a first one where quantum states are used through references and a second one where they are introduced as constants in the language. The quantum strategies presented in this thesis allow one to understand the constraints that must be imposed on quantum type systems with higher-order types. The most significant constraint is the fact that abstraction over part of the tensor product of many unknown quantum states must not be allowed. Quantum strategies are a new mathematical model which describes the interaction between classical and quantum data using system-environment dialogues. The interactions between the different parts of a quantum system are described using the rich structure generated by composition of strategies. This approach has enough generality to be put in relation with other
Visualizing hybridized quantum plasmons in coupled nanowires
DEFF Research Database (Denmark)
Andersen, Kirsten; Jensen, Kristian Lund; Mortensen, N. Asger
2013-01-01
of the dynamical dielectric function, which is computed using time-dependent density functional theory (TDDFT). For freestanding wires, the energy of both surface and bulk plasmon modes deviate from the classical result for low wire radii and high momentum transfer due to effects of electron spill-out, nonlocal......˚ separation, this mode is replaced by a charge-transfer plasmon, which blue shifts with decreasing separation in agreement with experiment and marks the onset of the strong tunneling regime....
Quantum optics of optomechanical networks
International Nuclear Information System (INIS)
Stannigel, K.
2012-01-01
This thesis proposes various setups in which micro-mechanical resonators and optomechanical systems can be combined with other quantum systems, such as solid-state qubits or atomic ensembles, in a beneficial way. These hybrid systems open up new ways for quantum control, and several protocols and applications for quantum information processing and, in particular, for quantum networks are presented. Part I describes an optically mediated coupling between the vibrational modes of a semi-transparent dielectric membrane and the center-of-mass motion of an atomic ensemble. Using the sophisticated toolbox available for the control of atomic systems, this setting enables an indirect manipulation of the membrane, including, for example, cooling it to the vibrational ground state. A fully quantum mechanical treatment of this open system is given in terms of the quantum stochastic Schrödinger equation. In Part II we explore the potential of optomechanical systems for quantum information processing applications. First, we introduce the concept of an optomechanical transducer, where a micro-mechanical resonator mediates an interaction between a solid-state based qubit on the one hand, and photons in an optical cavity on the other hand. The resulting qubit-light interface is shown to enable quantum state transfers between two distant solid-state qubits, thereby making them available for quantum networking applications. Second, we study multi-mode optomechanical systems in the single-photon single-phonon strong coupling regime. We predict quantum signatures of this interaction, which could be observed in future experiments, and provide a route towards possible applications of these systems as quantum information processing units. Part III presents a dissipative state preparation scheme for cascaded quantum networks. In such networks excitations can only propagate along a single spatial direction and the optomechanical transducer represents one way of realizing them. We show, in
Busch, Paul; Pellonpää, Juha-Pekka; Ylinen, Kari
2016-01-01
This is a book about the Hilbert space formulation of quantum mechanics and its measurement theory. It contains a synopsis of what became of the Mathematical Foundations of Quantum Mechanics since von Neumann’s classic treatise with this title. Fundamental non-classical features of quantum mechanics—indeterminacy and incompatibility of observables, unavoidable measurement disturbance, entanglement, nonlocality—are explicated and analysed using the tools of operational quantum theory. The book is divided into four parts: 1. Mathematics provides a systematic exposition of the Hilbert space and operator theoretic tools and relevant measure and integration theory leading to the Naimark and Stinespring dilation theorems; 2. Elements develops the basic concepts of quantum mechanics and measurement theory with a focus on the notion of approximate joint measurability; 3. Realisations offers in-depth studies of the fundamental observables of quantum mechanics and some of their measurement implementations; and 4....
Walls, D F
2007-01-01
Quantum Optics gives a comprehensive coverage of developments in quantum optics over the past years. In the early chapters the formalism of quantum optics is elucidated and the main techniques are introduced. These are applied in the later chapters to problems such as squeezed states of light, resonance fluorescence, laser theory, quantum theory of four-wave mixing, quantum non-demolition measurements, Bell's inequalities, and atom optics. Experimental results are used to illustrate the theory throughout. This yields the most comprehensive and up-to-date coverage of experiment and theory in quantum optics in any textbook. More than 40 exercises helps readers test their understanding and provide practice in quantitative problem solving.
International Nuclear Information System (INIS)
Markov, M.A.; West, P.C.
1984-01-01
This book discusses the state of the art of quantum gravity, quantum effects in cosmology, quantum black-hole physics, recent developments in supergravity, and quantum gauge theories. Topics considered include the problems of general relativity, pregeometry, complete cosmological theories, quantum fluctuations in cosmology and galaxy formation, a new inflationary universe scenario, grand unified phase transitions and the early Universe, the generalized second law of thermodynamics, vacuum polarization near black holes, the relativity of vacuum, black hole evaporations and their cosmological consequences, currents in supersymmetric theories, the Kaluza-Klein theories, gauge algebra and quantization, and twistor theory. This volume constitutes the proceedings of the Second Seminar on Quantum Gravity held in Moscow in 1981
Dutta, Debodyuti; Mishra, Sabyashachi
2017-07-27
The mechanism of the catalytic hydrolysis of N-succinyl diaminopimelic acid (SDAP) by the microbial enzyme DapE in its wild-type (wt) form as well as three of its mutants (E134D, H67A, and H349A) is investigated employing a hybrid quantum mechanics/molecular mechanics (QM/MM) method coupled with molecular dynamics (MD) simulations, wherein the time evolution of the atoms of the QM and MM regions are obtained from the forces acting on the individual atoms. The free-energy profiles along the reaction coordinates of this multistep hydrolysis reaction process are explored using a combination of equilibrium and nonequilibrium (umbrella sampling) QM/MM-MD simulation techniques. In the enzyme-substrate complexes of wt-DapE and the E134D mutant, nucleophilic attack is found to be the rate-determining step involving a barrier of 15.3 and 21.5 kcal/mol, respectively, which satisfactorily explains the free energy of activation obtained from kinetic experiments in wt-DapE-SDAP (15.2 kcal/mol) and the 3 orders of magnitude decrease in the catalytic activity due to E134D mutation. The catalysis is found to be quenched in the H67A and H349A mutants of DapE due to conformational rearrangement in the active site induced by the absence of the active site His residues that prohibits activation of the catalytic water molecule.
Stapp, Henry P.
2011-01-01
Robert Griffiths has recently addressed, within the framework of a 'consistent quantum theory' that he has developed, the issue of whether, as is often claimed, quantum mechanics entails a need for faster-than-light transfers of information over long distances. He argues that the putative proofs of this property that involve hidden variables include in their premises some essentially classical-physics-type assumptions that are fundamentally incompatible with the precepts of quantum physics. O...
Grifoni, Milena
1997-01-01
In this thesis, ratchet systems operating in the quantum regime are investigated. Ratchet systems, also known as Brownian motors, are periodic systems presenting an intrinsic asymmetry which can be exploited to extract work out of unbiased forces. As a model for ratchet systems, we consider the motion of a particle in a one-dimensional periodic and asymmetric potential, interacting with a thermal environment, and subject to an unbiased driving force. In quantum ratchets, intrinsic quantum flu...
Quantum space and quantum completeness
Jurić, Tajron
2018-05-01
Motivated by the question whether quantum gravity can "smear out" the classical singularity we analyze a certain quantum space and its quantum-mechanical completeness. Classical singularity is understood as a geodesic incompleteness, while quantum completeness requires a unique unitary time evolution for test fields propagating on an underlying background. Here the crucial point is that quantum completeness renders the Hamiltonian (or spatial part of the wave operator) to be essentially self-adjoint in order to generate a unique time evolution. We examine a model of quantum space which consists of a noncommutative BTZ black hole probed by a test scalar field. We show that the quantum gravity (noncommutative) effect is to enlarge the domain of BTZ parameters for which the relevant wave operator is essentially self-adjoint. This means that the corresponding quantum space is quantum complete for a larger range of BTZ parameters rendering the conclusion that in the quantum space one observes the effect of "smearing out" the singularity.
International Nuclear Information System (INIS)
Basdevant, J.L.; Dalibard, J.; Joffre, M.
2008-01-01
All physics is quantum from elementary particles to stars and to the big-bang via semi-conductors and chemistry. This theory is very subtle and we are not able to explain it without the help of mathematic tools. This book presents the principles of quantum mechanics and describes its mathematical formalism (wave function, Schroedinger equation, quantum operators, spin, Hamiltonians, collisions,..). We find numerous applications in the fields of new technologies (maser, quantum computer, cryptography,..) and in astrophysics. A series of about 90 exercises with their answers is included. This book is based on a physics course at a graduate level. (A.C.)
International Nuclear Information System (INIS)
Rodgers, P.
1998-01-01
There is more to information than a string of ones and zeroes the ability of ''quantum bits'' to be in two states at the same time could revolutionize information technology. In the mid-1930s two influential but seemingly unrelated papers were published. In 1935 Einstein, Podolsky and Rosen proposed the famous EPR paradox that has come to symbolize the mysteries of quantum mechanics. Two years later, Alan Turing introduced the universal Turing machine in an enigmatically titled paper, On computable numbers, and laid the foundations of the computer industry one of the biggest industries in the world today. Although quantum physics is essential to understand the operation of transistors and other solid-state devices in computers, computation itself has remained a resolutely classical process. Indeed it seems only natural that computation and quantum theory should be kept as far apart as possible surely the uncertainty associated with quantum theory is anathema to the reliability expected from computers? Wrong. In 1985 David Deutsch introduced the universal quantum computer and showed that quantum theory can actually allow computers to do more rather than less. The ability of particles to be in a superposition of more than one quantum state naturally introduces a form of parallelism that can, in principle, perform some traditional computing tasks faster than is possible with classical computers. Moreover, quantum computers are capable of other tasks that are not conceivable with their classical counterparts. Similar breakthroughs in cryptography and communication followed. (author)
Energy Technology Data Exchange (ETDEWEB)
Rodgers, P
1998-03-01
There is more to information than a string of ones and zeroes the ability of ''quantum bits'' to be in two states at the same time could revolutionize information technology. In the mid-1930s two influential but seemingly unrelated papers were published. In 1935 Einstein, Podolsky and Rosen proposed the famous EPR paradox that has come to symbolize the mysteries of quantum mechanics. Two years later, Alan Turing introduced the universal Turing machine in an enigmatically titled paper, On computable numbers, and laid the foundations of the computer industry one of the biggest industries in the world today. Although quantum physics is essential to understand the operation of transistors and other solid-state devices in computers, computation itself has remained a resolutely classical process. Indeed it seems only natural that computation and quantum theory should be kept as far apart as possible surely the uncertainty associated with quantum theory is anathema to the reliability expected from computers? Wrong. In 1985 David Deutsch introduced the universal quantum computer and showed that quantum theory can actually allow computers to do more rather than less. The ability of particles to be in a superposition of more than one quantum state naturally introduces a form of parallelism that can, in principle, perform some traditional computing tasks faster than is possible with classical computers. Moreover, quantum computers are capable of other tasks that are not conceivable with their classical counterparts. Similar breakthroughs in cryptography and communication followed. (author)
International Nuclear Information System (INIS)
Khrennikov, Andrei; Klein, Moshe; Mor, Tal
2010-01-01
In number theory, a partition of a positive integer n is a way of writing n as a sum of positive integers. The number of partitions of n is given by the partition function p(n). Inspired by quantum information processing, we extend the concept of partitions in number theory as follows: for an integer n, we treat each partition as a basis state of a quantum system representing that number n, so that the Hilbert-space that corresponds to that integer n is of dimension p(n); the 'classical integer' n can thus be generalized into a (pure) quantum state ||ψ(n) > which is a superposition of the partitions of n, in the same way that a quantum bit (qubit) is a generalization of a classical bit. More generally, ρ(n) is a density matrix in that same Hilbert-space (a probability distribution over pure states). Inspired by the notion of quantum numbers in quantum theory (such as in Bohr's model of the atom), we then try to go beyond the partitions, by defining (via recursion) the notion of 'sub-partitions' in number theory. Combining the two notions mentioned above, sub-partitions and quantum integers, we finally provide an alternative definition of the quantum integers [the pure-state |ψ'(n)> and the mixed-state ρ'(n),] this time using the sub-partitions as the basis states instead of the partitions, for describing the quantum number that corresponds to the integer n.
International Nuclear Information System (INIS)
Deutsch, D.
1992-01-01
As computers become ever more complex, they inevitably become smaller. This leads to a need for components which are fabricated and operate on increasingly smaller size scales. Quantum theory is already taken into account in microelectronics design. This article explores how quantum theory will need to be incorporated into computers in future in order to give them their components functionality. Computation tasks which depend on quantum effects will become possible. Physicists may have to reconsider their perspective on computation in the light of understanding developed in connection with universal quantum computers. (UK)
Energy Technology Data Exchange (ETDEWEB)
Rodgers, P
1998-03-01
There is more to information than a string of ones and zeroes the ability of ''quantum bits'' to be in two states at the same time could revolutionize information technology. In the mid-1930s two influential but seemingly unrelated papers were published. In 1935 Einstein, Podolsky and Rosen proposed the famous EPR paradox that has come to symbolize the mysteries of quantum mechanics. Two years later, Alan Turing introduced the universal Turing machine in an enigmatically titled paper, On computable numbers, and laid the foundations of the computer industry one of the biggest industries in the world today. Although quantum physics is essential to understand the operation of transistors and other solid-state devices in computers, computation itself has remained a resolutely classical process. Indeed it seems only natural that computation and quantum theory should be kept as far apart as possible surely the uncertainty associated with quantum theory is anathema to the reliability expected from computers? Wrong. In 1985 David Deutsch introduced the universal quantum computer and showed that quantum theory can actually allow computers to do more rather than less. The ability of particles to be in a superposition of more than one quantum state naturally introduces a form of parallelism that can, in principle, perform some traditional computing tasks faster than is possible with classical computers. Moreover, quantum computers are capable of other tasks that are not conceivable with their classical counterparts. Similar breakthroughs in cryptography and communication followed. (author)
Tartakovskii, Alexander
2012-07-01
Part I. Nanostructure Design and Structural Properties of Epitaxially Grown Quantum Dots and Nanowires: 1. Growth of III/V semiconductor quantum dots C. Schneider, S. Hofling and A. Forchel; 2. Single semiconductor quantum dots in nanowires: growth, optics, and devices M. E. Reimer, N. Akopian, M. Barkelid, G. Bulgarini, R. Heeres, M. Hocevar, B. J. Witek, E. Bakkers and V. Zwiller; 3. Atomic scale analysis of self-assembled quantum dots by cross-sectional scanning tunneling microscopy and atom probe tomography J. G. Keizer and P. M. Koenraad; Part II. Manipulation of Individual Quantum States in Quantum Dots Using Optical Techniques: 4. Studies of the hole spin in self-assembled quantum dots using optical techniques B. D. Gerardot and R. J. Warburton; 5. Resonance fluorescence from a single quantum dot A. N. Vamivakas, C. Matthiesen, Y. Zhao, C.-Y. Lu and M. Atature; 6. Coherent control of quantum dot excitons using ultra-fast optical techniques A. J. Ramsay and A. M. Fox; 7. Optical probing of holes in quantum dot molecules: structure, symmetry, and spin M. F. Doty and J. I. Climente; Part III. Optical Properties of Quantum Dots in Photonic Cavities and Plasmon-Coupled Dots: 8. Deterministic light-matter coupling using single quantum dots P. Senellart; 9. Quantum dots in photonic crystal cavities A. Faraon, D. Englund, I. Fushman, A. Majumdar and J. Vukovic; 10. Photon statistics in quantum dot micropillar emission M. Asmann and M. Bayer; 11. Nanoplasmonics with colloidal quantum dots V. Temnov and U. Woggon; Part IV. Quantum Dot Nano-Laboratory: Magnetic Ions and Nuclear Spins in a Dot: 12. Dynamics and optical control of an individual Mn spin in a quantum dot L. Besombes, C. Le Gall, H. Boukari and H. Mariette; 13. Optical spectroscopy of InAs/GaAs quantum dots doped with a single Mn atom O. Krebs and A. Lemaitre; 14. Nuclear spin effects in quantum dot optics B. Urbaszek, B. Eble, T. Amand and X. Marie; Part V. Electron Transport in Quantum Dots Fabricated by
Quantum group and quantum symmetry
International Nuclear Information System (INIS)
Chang Zhe.
1994-05-01
This is a self-contained review on the theory of quantum group and its applications to modern physics. A brief introduction is given to the Yang-Baxter equation in integrable quantum field theory and lattice statistical physics. The quantum group is primarily introduced as a systematic method for solving the Yang-Baxter equation. Quantum group theory is presented within the framework of quantum double through quantizing Lie bi-algebra. Both the highest weight and the cyclic representations are investigated for the quantum group and emphasis is laid on the new features of representations for q being a root of unity. Quantum symmetries are explored in selected topics of modern physics. For a Hamiltonian system the quantum symmetry is an enlarged symmetry that maintains invariance of equations of motion and allows a deformation of the Hamiltonian and symplectic form. The configuration space of the integrable lattice model is analyzed in terms of the representation theory of quantum group. By means of constructing the Young operators of quantum group, the Schroedinger equation of the model is transformed to be a set of coupled linear equations that can be solved by the standard method. Quantum symmetry of the minimal model and the WZNW model in conformal field theory is a hidden symmetry expressed in terms of screened vertex operators, and has a deep interplay with the Virasoro algebra. In quantum group approach a complete description for vibrating and rotating diatomic molecules is given. The exact selection rules and wave functions are obtained. The Taylor expansion of the analytic formulas of the approach reproduces the famous Dunham expansion. (author). 133 refs, 20 figs
Quantum information. Teleportation - cryptography - quantum computer
International Nuclear Information System (INIS)
Koenneker, Carsten
2012-01-01
The following topics are dealt with: Reality in the test facility, quantum teleportation, the reality of quanta, interaction-free quantum measurement, rules for quantum computers, quantum computers with ions, spintronics with diamond, the limits of the quantum computers, a view in the future of quantum optics. (HSI)
Quantum ensembles of quantum classifiers.
Schuld, Maria; Petruccione, Francesco
2018-02-09
Quantum machine learning witnesses an increasing amount of quantum algorithms for data-driven decision making, a problem with potential applications ranging from automated image recognition to medical diagnosis. Many of those algorithms are implementations of quantum classifiers, or models for the classification of data inputs with a quantum computer. Following the success of collective decision making with ensembles in classical machine learning, this paper introduces the concept of quantum ensembles of quantum classifiers. Creating the ensemble corresponds to a state preparation routine, after which the quantum classifiers are evaluated in parallel and their combined decision is accessed by a single-qubit measurement. This framework naturally allows for exponentially large ensembles in which - similar to Bayesian learning - the individual classifiers do not have to be trained. As an example, we analyse an exponentially large quantum ensemble in which each classifier is weighed according to its performance in classifying the training data, leading to new results for quantum as well as classical machine learning.
Quantum computer games: quantum minesweeper
Gordon, Michal; Gordon, Goren
2010-07-01
The computer game of quantum minesweeper is introduced as a quantum extension of the well-known classical minesweeper. Its main objective is to teach the unique concepts of quantum mechanics in a fun way. Quantum minesweeper demonstrates the effects of superposition, entanglement and their non-local characteristics. While in the classical minesweeper the goal of the game is to discover all the mines laid out on a board without triggering them, in the quantum version there are several classical boards in superposition. The goal is to know the exact quantum state, i.e. the precise layout of all the mines in all the superposed classical boards. The player can perform three types of measurement: a classical measurement that probabilistically collapses the superposition; a quantum interaction-free measurement that can detect a mine without triggering it; and an entanglement measurement that provides non-local information. The application of the concepts taught by quantum minesweeper to one-way quantum computing are also presented.
Quantum Physics Without Quantum Philosophy
Dürr, Detlef; Zanghì, Nino
2013-01-01
It has often been claimed that without drastic conceptual innovations a genuine explanation of quantum interference effects and quantum randomness is impossible. This book concerns Bohmian mechanics, a simple particle theory that is a counterexample to such claims. The gentle introduction and other contributions collected here show how the phenomena of non-relativistic quantum mechanics, from Heisenberg's uncertainty principle to non-commuting observables, emerge from the Bohmian motion of particles, the natural particle motion associated with Schrödinger's equation. This book will be of value to all students and researchers in physics with an interest in the meaning of quantum theory as well as to philosophers of science.
Quantum measurement in quantum optics
International Nuclear Information System (INIS)
Kimble, H.J.
1993-01-01
Recent progress in the generation and application of manifestly quantum or nonclassical states of the electromagnetic field is reviewed with emphasis on the research of the Quantum Optics Group at Caltech. In particular, the possibilities for spectroscopy with non-classical light are discussed both in terms of improved quantitative measurement capabilities and for the fundamental alteration of atomic radiative processes. Quantum correlations for spatially extended systems are investigated in a variety of experiments which utilize nondegenerate parametric down conversion. Finally, the prospects for measurement of the position of a free mass with precision beyond the standard quantum limit are briefly considered. (author). 38 refs., 1 fig
Indian Academy of Sciences (India)
Home; Journals; Resonance – Journal of Science Education; Volume 5; Issue 9. Quantum Computing - Building Blocks of a Quantum Computer. C S Vijay Vishal Gupta. General Article Volume 5 Issue 9 September 2000 pp 69-81. Fulltext. Click here to view fulltext PDF. Permanent link:
International Nuclear Information System (INIS)
Doplicher, S.
1996-01-01
We review some recent result and work in progress on the quantum structure of spacetime at scales comparable with the Planck length; the models discussed here are operationally motivated by the limitations in the accuracy of localization of events in spacetime imposed by the interplay between quantum mechanics and classical general relativity. (orig.)
Quantum Accelerators for High-Performance Computing Systems
Britt, Keith A.; Mohiyaddin, Fahd A.; Humble, Travis S.
2017-01-01
We define some of the programming and system-level challenges facing the application of quantum processing to high-performance computing. Alongside barriers to physical integration, prominent differences in the execution of quantum and conventional programs challenges the intersection of these computational models. Following a brief overview of the state of the art, we discuss recent advances in programming and execution models for hybrid quantum-classical computing. We discuss a novel quantu...
Pearsall, Thomas P
2017-01-01
This textbook employs a pedagogical approach that facilitates access to the fundamentals of Quantum Photonics. It contains an introductory description of the quantum properties of photons through the second quantization of the electromagnetic field, introducing stimulated and spontaneous emission of photons at the quantum level. Schrödinger’s equation is used to describe the behavior of electrons in a one-dimensional potential. Tunneling through a barrier is used to introduce the concept of nonlocality of an electron at the quantum level, which is closely-related to quantum confinement tunneling, resonant tunneling, and the origin of energy bands in both periodic (crystalline) and aperiodic (non-crystalline) materials. Introducing the concepts of reciprocal space, Brillouin zones, and Bloch’s theorem, the determination of electronic band structure using the pseudopotential method is presented, allowing direct computation of the band structures of most group IV, group III-V, and group II-VI semiconducto...
International Nuclear Information System (INIS)
Hawking, S.W.
1984-01-01
The subject of these lectures is quantum effects in cosmology. The author deals first with situations in which the gravitational field can be treated as a classical, unquantized background on which the quantum matter fields propagate. This is the case with inflation at the GUT era. Nevertheless the curvature of spacetime can have important effects on the behaviour of the quantum fields and on the development of long-range correlations. He then turns to the question of the quantization of the gravitational field itself. The plan of these lectures is as follows: Euclidean approach to quantum field theory in flat space; the extension of techniques to quantum fields on a curved background with the four-sphere, the Euclidean version of De Sitter space as a particular example; the GUT era; quantization of the gravitational field by Euclidean path integrals; mini superspace model. (Auth.)
Rae, Alastair I M
2016-01-01
A Thorough Update of One of the Most Highly Regarded Textbooks on Quantum Mechanics Continuing to offer an exceptionally clear, up-to-date treatment of the subject, Quantum Mechanics, Sixth Edition explains the concepts of quantum mechanics for undergraduate students in physics and related disciplines and provides the foundation necessary for other specialized courses. This sixth edition builds on its highly praised predecessors to make the text even more accessible to a wider audience. It is now divided into five parts that separately cover broad topics suitable for any general course on quantum mechanics. New to the Sixth Edition * Three chapters that review prerequisite physics and mathematics, laying out the notation, formalism, and physical basis necessary for the rest of the book * Short descriptions of numerous applications relevant to the physics discussed, giving students a brief look at what quantum mechanics has made possible industrially and scientifically * Additional end-of-chapter problems with...
Richter, Johannes; Farnell, Damian; Bishop, Raymod
2004-01-01
The investigation of magnetic systems where quantum effects play a dominant role has become a very active branch of solid-state-physics research in its own right. The first three chapters of the "Quantum Magnetism" survey conceptual problems and provide insights into the classes of systems considered, namely one-dimensional, two-dimensional and molecular magnets. The following chapters introduce the methods used in the field of quantum magnetism, including spin wave analysis, exact diagonalization, quantum field theory, coupled cluster methods and the Bethe ansatz. The book closes with a chapter on quantum phase transitions and a contribution that puts the wealth of phenomena into the context of experimental solid-state physics. Closing a gap in the literature, this volume is intended both as an introductory text at postgraduate level and as a modern, comprehensive reference for researchers in the field.
Coherence protection in coupled quantum systems
Cammack, H. M.; Kirton, P.; Stace, T. M.; Eastham, P. R.; Keeling, J.; Lovett, B. W.
2018-02-01
The interaction of a quantum system with its environment causes decoherence, setting a fundamental limit on its suitability for quantum information processing. However, we show that if the system consists of coupled parts with different internal energy scales then the interaction of one part with a thermal bath need not lead to loss of coherence from the other. Remarkably, we find that the protected part can remain coherent for longer when the coupling to the bath becomes stronger or the temperature is raised. Our theory will enable the design of decoherence-resistant hybrid quantum computers.
International Nuclear Information System (INIS)
Steane, Andrew
1998-01-01
The subject of quantum computing brings together ideas from classical information theory, computer science, and quantum physics. This review aims to summarize not just quantum computing, but the whole subject of quantum information theory. Information can be identified as the most general thing which must propagate from a cause to an effect. It therefore has a fundamentally important role in the science of physics. However, the mathematical treatment of information, especially information processing, is quite recent, dating from the mid-20th century. This has meant that the full significance of information as a basic concept in physics is only now being discovered. This is especially true in quantum mechanics. The theory of quantum information and computing puts this significance on a firm footing, and has led to some profound and exciting new insights into the natural world. Among these are the use of quantum states to permit the secure transmission of classical information (quantum cryptography), the use of quantum entanglement to permit reliable transmission of quantum states (teleportation), the possibility of preserving quantum coherence in the presence of irreversible noise processes (quantum error correction), and the use of controlled quantum evolution for efficient computation (quantum computation). The common theme of all these insights is the use of quantum entanglement as a computational resource. It turns out that information theory and quantum mechanics fit together very well. In order to explain their relationship, this review begins with an introduction to classical information theory and computer science, including Shannon's theorem, error correcting codes, Turing machines and computational complexity. The principles of quantum mechanics are then outlined, and the Einstein, Podolsky and Rosen (EPR) experiment described. The EPR-Bell correlations, and quantum entanglement in general, form the essential new ingredient which distinguishes quantum from
Energy Technology Data Exchange (ETDEWEB)
Steane, Andrew [Department of Atomic and Laser Physics, University of Oxford, Clarendon Laboratory, Oxford (United Kingdom)
1998-02-01
The subject of quantum computing brings together ideas from classical information theory, computer science, and quantum physics. This review aims to summarize not just quantum computing, but the whole subject of quantum information theory. Information can be identified as the most general thing which must propagate from a cause to an effect. It therefore has a fundamentally important role in the science of physics. However, the mathematical treatment of information, especially information processing, is quite recent, dating from the mid-20th century. This has meant that the full significance of information as a basic concept in physics is only now being discovered. This is especially true in quantum mechanics. The theory of quantum information and computing puts this significance on a firm footing, and has led to some profound and exciting new insights into the natural world. Among these are the use of quantum states to permit the secure transmission of classical information (quantum cryptography), the use of quantum entanglement to permit reliable transmission of quantum states (teleportation), the possibility of preserving quantum coherence in the presence of irreversible noise processes (quantum error correction), and the use of controlled quantum evolution for efficient computation (quantum computation). The common theme of all these insights is the use of quantum entanglement as a computational resource. It turns out that information theory and quantum mechanics fit together very well. In order to explain their relationship, this review begins with an introduction to classical information theory and computer science, including Shannon's theorem, error correcting codes, Turing machines and computational complexity. The principles of quantum mechanics are then outlined, and the Einstein, Podolsky and Rosen (EPR) experiment described. The EPR-Bell correlations, and quantum entanglement in general, form the essential new ingredient which distinguishes quantum from
Quantum dots and nanocomposites.
Mansur, Herman Sander
2010-01-01
Quantum dots (QDs), also known as semiconducting nanoparticles, are promising zero-dimensional advanced materials because of their nanoscale size and because they can be engineered to suit particular applications such as nonlinear optical devices (NLO), electro-optical devices, and computing applications. QDs can be joined to polymers in order to produce nanocomposites which can be considered a scientific revolution of the 21st century. One of the fastest moving and most exciting interfaces of nanotechnology is the use of QDs in medicine, cell and molecular biology. Recent advances in nanomaterials have produced a new class of markers and probes by conjugating semiconductor QDs with biomolecules that have affinities for binding with selected biological structures. The nanoscale of QDs ensures that they do not scatter light at visible or longer wavelengths, which is important in order to minimize optical losses in practical applications. Moreover, at this scale, quantum confinement and surface effects become very important and therefore manipulation of the dot diameter or modification of its surface allows the properties of the dot to be controlled. Quantum confinement affects the absorption and emission of photons from the dot. Thus, the absorption edge of a material can be tuned by control of the particle size. This paper reviews developments in the myriad of possibilities for the use of semiconductor QDs associated with molecules producing novel hybrid nanocomposite systems for nanomedicine and bioengineering applications.
Quantum Accelerators for High-performance Computing Systems
Energy Technology Data Exchange (ETDEWEB)
Humble, Travis S. [ORNL; Britt, Keith A. [ORNL; Mohiyaddin, Fahd A. [ORNL
2017-11-01
We define some of the programming and system-level challenges facing the application of quantum processing to high-performance computing. Alongside barriers to physical integration, prominent differences in the execution of quantum and conventional programs challenges the intersection of these computational models. Following a brief overview of the state of the art, we discuss recent advances in programming and execution models for hybrid quantum-classical computing. We discuss a novel quantum-accelerator framework that uses specialized kernels to offload select workloads while integrating with existing computing infrastructure. We elaborate on the role of the host operating system to manage these unique accelerator resources, the prospects for deploying quantum modules, and the requirements placed on the language hierarchy connecting these different system components. We draw on recent advances in the modeling and simulation of quantum computing systems with the development of architectures for hybrid high-performance computing systems and the realization of software stacks for controlling quantum devices. Finally, we present simulation results that describe the expected system-level behavior of high-performance computing systems composed from compute nodes with quantum processing units. We describe performance for these hybrid systems in terms of time-to-solution, accuracy, and energy consumption, and we use simple application examples to estimate the performance advantage of quantum acceleration.
Quantum mechanics with quantum time
International Nuclear Information System (INIS)
Kapuscik, E.
1984-01-01
Using a non-canonical Lie structure of classical mechanics a new algebra of quantum mechanical observables is constructed. The new algebra, in addition to the notion of classical time, makes it possible to introduce the notion of quantum time. A new type of uncertainty relation is derived. (author)
Natural and artificial atoms for quantum computation
Energy Technology Data Exchange (ETDEWEB)
Buluta, Iulia; Ashhab, Sahel; Nori, Franco, E-mail: fnori@riken.jp [Advanced Science Institute, RIKEN, Wako-shi, Saitama, 351-0198 (Japan)
2011-10-15
Remarkable progress towards realizing quantum computation has been achieved using natural and artificial atoms as qubits. This paper presents a brief overview of the current status of different types of qubits. On the one hand, natural atoms (such as neutral atoms and ions) have long coherence times, and could be stored in large arrays, providing ideal 'quantum memories'. On the other hand, artificial atoms (such as superconducting circuits or semiconductor quantum dots) have the advantage of custom-designed features and could be used as 'quantum processing units'. Natural and artificial atoms can be coupled with each other and can also be interfaced with photons for long-distance communications. Hybrid devices made of natural/artificial atoms and photons may provide the next-generation design for quantum computers.