Ultrafast Electron Dynamics in Solar Energy Conversion.

Science.gov (United States)

Ponseca, Carlito S; Chábera, Pavel; Uhlig, Jens; Persson, Petter; Sundström, Villy

2017-08-23

Electrons are the workhorses of solar energy conversion. Conversion of the energy of light to electricity in photovoltaics, or to energy-rich molecules (solar fuel) through photocatalytic processes, invariably starts with photoinduced generation of energy-rich electrons. The harvesting of these electrons in practical devices rests on a series of electron transfer processes whose dynamics and efficiencies determine the function of materials and devices. To capture the energy of a photogenerated electron-hole pair in a solar cell material, charges of opposite sign have to be separated against electrostatic attractions, prevented from recombining and being transported through the active material to electrodes where they can be extracted. In photocatalytic solar fuel production, these electron processes are coupled to chemical reactions leading to storage of the energy of light in chemical bonds. With the focus on the ultrafast time scale, we here discuss the light-induced electron processes underlying the function of several molecular and hybrid materials currently under development for solar energy applications in dye or quantum dot-sensitized solar cells, polymer-fullerene polymer solar cells, organometal halide perovskite solar cells, and finally some photocatalytic systems.

Ultrafast Photoinduced Electron Transfer in a π-Conjugated Oligomer/Porphyrin Complex

KAUST Repository

Aly, Shawkat Mohammede; Goswami, Subhadip; Alsulami, Qana; Schanze, Kirk S.; Mohammed, Omar F.

2014-01-01

Controlling charge transfer (CT), charge separation (CS), and charge recombination (CR) at the donor-acceptor interface is extremely important to optimize the conversion efficiency in solar cell devices. In general, ultrafast CT and slow CR

Direct observation of the ultrafast electron transfer process in a polymer/fullerene blend

NARCIS (Netherlands)

Cerullo, G.; Lanzani, G.; Silvestri, S. De; Brabec, Ch.J.; Zerza, G.; Sariciftci, N.S.; Hummelen, J.C.

2000-01-01

Photoinduced electron transfer in organic molecules is an extensively investigated topic both because of fundamental interest in the photophysics and for applications to artificial photosynthesis. Highly efficient ultrafast electron transfer from photoexcited conjugated polymers to C60 has been

Carotenoid-to-bacteriochlorophyll energy transfer through vibronic coupling in LH2 from Phaeosprillum molischianum.

Science.gov (United States)

Thyrhaug, Erling; Lincoln, Craig N; Branchi, Federico; Cerullo, Giulio; Perlík, Václav; Šanda, František; Lokstein, Heiko; Hauer, Jürgen

2018-03-01

The peripheral light-harvesting antenna complex (LH2) of purple photosynthetic bacteria is an ideal testing ground for models of structure-function relationships due to its well-determined molecular structure and ultrafast energy deactivation. It has been the target for numerous studies in both theory and ultrafast spectroscopy; nevertheless, certain aspects of the convoluted relaxation network of LH2 lack a satisfactory explanation by conventional theories. For example, the initial carotenoid-to-bacteriochlorophyll energy transfer step necessary on visible light excitation was long considered to follow the Förster mechanism, even though transfer times as short as 40 femtoseconds (fs) have been observed. Such transfer times are hard to accommodate by Förster theory, as the moderate coupling strengths found in LH2 suggest much slower transfer within this framework. In this study, we investigate LH2 from Phaeospirillum (Ph.) molischianum in two types of transient absorption experiments-with narrowband pump and white-light probe resulting in 100 fs time resolution, and with degenerate broadband 10 fs pump and probe pulses. With regard to the split Q x band in this system, we show that vibronically mediated transfer explains both the ultrafast carotenoid-to-B850 transfer, and the almost complete lack of transfer to B800. These results are beyond Förster theory, which predicts an almost equal partition between the two channels.

Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation.

Science.gov (United States)

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho, Jr-Wei; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-28

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH 3 ) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH 3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S 1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH 3 ] + cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ∼70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.

Ultrafast excitation energy transfer from encapsulated quaterrylene to single-walled carbon nanotube

Energy Technology Data Exchange (ETDEWEB)

Koyama, Takeshi, E-mail: koyama@nuap.nagoya-u.ac.jp [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Tsunekawa, Takuya [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Saito, Takeshi [Research Center for Advanced Carbon Materials, AIST, Tsukuba, Ibaraki 305-8565 (Japan); Asaka, Koji; Saito, Yahachi [Department of Quantum Engineering, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Kishida, Hideo [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Nakamura, Arao [Department of Applied Physics, Nagoya University, Chikusa, Nagoya 464-8603 (Japan); Toyota Physical and Chemical Research Institute, Nagakute, Aichi 480-1192 (Japan)

2016-01-15

We investigate excitation energy transfer from an encapsulated quaterrylene molecule to a single-walled carbon nanotube by means of femtosecond pump-probe spectroscopy. The time constant of energy transfer becomes shorter with increasing average diameter of nanotube: 1.4±0.2 ps for 1.0 nm, 1.1±0.2 ps for 1.4 nm, and 0.4±0.1 ps for 1.8 nm. The observed behavior is discussed considering the distance of less than 1 nm between the molecule and the nanotube wall. - Highlights: • Dynamical properties of excited states in quaterrylene/SWNT composites were studied. • Excitation energy transfer occurs in the time range of 0.4-1.4 ps. • The transfer rate depends on the nanotube diameter, i.e. molecule-nanotube wall distance. • This dependence indicates the feature of excitation energy transfer on the nanoscale.

Ultrafast Photoinduced Electron Transfer in a π-Conjugated Oligomer/Porphyrin Complex

KAUST Repository

Aly, Shawkat Mohammede

2014-10-02

Controlling charge transfer (CT), charge separation (CS), and charge recombination (CR) at the donor-acceptor interface is extremely important to optimize the conversion efficiency in solar cell devices. In general, ultrafast CT and slow CR are desirable for optimal device performance. In this Letter, the ultrafast excited-state CT between platinum oligomer (DPP-Pt(acac)) as a new electron donor and porphyrin as an electron acceptor is monitored for the first time using femtosecond (fs) transient absorption (TA) spectroscopy with broad-band capability and 120 fs temporal resolution. Turning the CT on/off has been shown to be possible either by switching from an organometallic oligomer to a metal-free oligomer or by controlling the charge density on the nitrogen atom of the porphyrin meso unit. Our time-resolved data show that the CT and CS between DPP-Pt(acac) and cationic porphyrin are ultrafast (approximately 1.5 ps), and the CR is slow (ns time scale), as inferred from the formation and the decay of the cationic and anionic species. We also found that the metallic center in the DPP-Pt(acac) oligomer and the positive charge on the porphyrin are the keys to switching on/off the ultrafast CT process.

Optimal and robust control of quantum state transfer by shaping the spectral phase of ultrafast laser pulses.

Science.gov (United States)

Guo, Yu; Dong, Daoyi; Shu, Chuan-Cun

2018-04-04

Achieving fast and efficient quantum state transfer is a fundamental task in physics, chemistry and quantum information science. However, the successful implementation of the perfect quantum state transfer also requires robustness under practically inevitable perturbative defects. Here, we demonstrate how an optimal and robust quantum state transfer can be achieved by shaping the spectral phase of an ultrafast laser pulse in the framework of frequency domain quantum optimal control theory. Our numerical simulations of the single dibenzoterrylene molecule as well as in atomic rubidium show that optimal and robust quantum state transfer via spectral phase modulated laser pulses can be achieved by incorporating a filtering function of the frequency into the optimization algorithm, which in turn has potential applications for ultrafast robust control of photochemical reactions.

Direct observation of multistep energy transfer in LHCII with fifth-order 3D electronic spectroscopy.

Science.gov (United States)

Zhang, Zhengyang; Lambrev, Petar H; Wells, Kym L; Garab, Győző; Tan, Howe-Siang

2015-07-31

During photosynthesis, sunlight is efficiently captured by light-harvesting complexes, and the excitation energy is then funneled towards the reaction centre. These photosynthetic excitation energy transfer (EET) pathways are complex and proceed in a multistep fashion. Ultrafast two-dimensional electronic spectroscopy (2DES) is an important tool to study EET processes in photosynthetic complexes. However, the multistep EET processes can only be indirectly inferred by correlating different cross peaks from a series of 2DES spectra. Here we directly observe multistep EET processes in LHCII using ultrafast fifth-order three-dimensional electronic spectroscopy (3DES). We measure cross peaks in 3DES spectra of LHCII that directly indicate energy transfer from excitons in the chlorophyll b (Chl b) manifold to the low-energy level chlorophyll a (Chl a) via mid-level Chl a energy states. This new spectroscopic technique allows scientists to move a step towards mapping the complete complex EET processes in photosynthetic systems.

Ultrafast quenching of tryptophan fluorescence in proteins: Interresidue and intrahelical electron transfer

Energy Technology Data Exchange (ETDEWEB)

Qiu Weihong; Li Tanping; Zhang Luyuan; Yang Yi; Kao Yating; Wang Lijuan [Department of Physics, Chemistry, and Biochemistry, Program of Biophysics, Chemical Physics, and Biochemistry, Ohio State University, Columbus, OH 43210 (United States); Zhong Dongping [Department of Physics, Chemistry, and Biochemistry, Program of Biophysics, Chemical Physics, and Biochemistry, Ohio State University, Columbus, OH 43210 (United States)], E-mail: dongping@mps.ohio-state.edu

2008-06-23

Quenching of tryptophan fluorescence in proteins has been critical to the understanding of protein dynamics and enzyme reactions using tryptophan as a molecular optical probe. We report here our systematic examinations of potential quenching residues with more than 40 proteins. With site-directed mutation, we placed tryptophan to desired positions or altered its neighboring residues to screen quenching groups among 20 amino acid residues and of peptide backbones. With femtosecond resolution, we observed the ultrafast quenching dynamics within 100 ps and identified two ultrafast quenching groups, the carbonyl- and sulfur-containing residues. The former is glutamine and glutamate residues and the later is disulfide bond and cysteine residue. The quenching by the peptide-bond carbonyl group as well as other potential residues mostly occurs in longer than 100 ps. These ultrafast quenching dynamics occur at van der Waals distances through intraprotein electron transfer with high directionality. Following optimal molecular orbital overlap, electron jumps from the benzene ring of the indole moiety in a vertical orientation to the LUMO of acceptor quenching residues. Molecular dynamics simulations were invoked to elucidate various correlations of quenching dynamics with separation distances, relative orientations, local fluctuations and reaction heterogeneity. These unique ultrafast quenching pairs, as recently found to extensively occur in high-resolution protein structures, may have significant biological implications.

Ultrafast modulation of near-field heat transfer with tunable metamaterials

OpenAIRE

Cui, Longji; Huang, Yong; Wang, Ju; Zhu, Ke-Yong

2012-01-01

We propose a mechanism of active near-field heat transfer modulation relying on externally tunable metamaterials. A large modulation effect is observed and can be explained by the coupling of surface modes, which is dramatically varied in the presence of controllable magnetoelectric coupling in metamaterials. We finally discuss how a practical picosecond-scale thermal modulator can be made. This modulator allows manipulating nanoscale heat flux in an ultrafast and noncontact (by optical means...

Imaging and Manipulating Energy Transfer Among Quantum Dots at Individual Dot Resolution.

Science.gov (United States)

Nguyen, Duc; Nguyen, Huy A; Lyding, Joseph W; Gruebele, Martin

2017-06-27

Many processes of interest in quantum dots involve charge or energy transfer from one dot to another. Energy transfer in films of quantum dots as well as between linked quantum dots has been demonstrated by luminescence shift, and the ultrafast time-dependence of energy transfer processes has been resolved. Bandgap variation among dots (energy disorder) and dot separation are known to play an important role in how energy diffuses. Thus, it would be very useful if energy transfer could be visualized directly on a dot-by-dot basis among small clusters or within films of quantum dots. To that effect, we report single molecule optical absorption detected by scanning tunneling microscopy (SMA-STM) to image energy pooling from donor into acceptor dots on a dot-by-dot basis. We show that we can manipulate groups of quantum dots by pruning away the dominant acceptor dot, and switching the energy transfer path to a different acceptor dot. Our experimental data agrees well with a simple Monte Carlo lattice model of energy transfer, similar to models in the literature, in which excitation energy is transferred preferentially from dots with a larger bandgap to dots with a smaller bandgap.

Ultra-Fast Low Energy Switching Using an InP Photonic Crystal H0 Nanocavity

DEFF Research Database (Denmark)

Yu, Yi; Palushani, Evarist; Heuck, Mikkel

2013-01-01

Pump-probe measurements on InP photonic crystal H0 nanocavities show large-contrast ultrafast switching at low pulse energy. For large pulse energies, high-frequency carrier density oscillations are induced, leading to pulsesplitting.......Pump-probe measurements on InP photonic crystal H0 nanocavities show large-contrast ultrafast switching at low pulse energy. For large pulse energies, high-frequency carrier density oscillations are induced, leading to pulsesplitting....

Femtosecond pump probe spectroscopy for the study of energy transfer of light-harvesting complexes from extractions of spinach leaves

Directory of Open Access Journals (Sweden)

L. van Rensburg

2010-01-01

Full Text Available Measurements of ultrafast transient processes, of temporal durations in the picosecond and femtosecond regime, are made possible by femtosecond pump probe transient absorption spectroscopy. Such an ultrafast pump probe transient absorption setup has been implemented at the CSIR National Laser Centre and has been applied to investigate energy transfer processes in different parts of photosynthetic systems. In this paper we report on our first results obtained with Malachite green as a benchmark. Malachite green was chosen because the lifetime of its excited state is well known. We also present experimental results of the ultrafast energy transfer of light-harvesting complexes in samples prepared from spinach leaves. Various pump wavelengths in the range 600–680 nm were used; the probe was a white light continuum spanning 420–700 nm. The experimental setup is described in detail in this paper. Results obtained with these samples are consistent with those expected and achieved by other researchers in this field.

Energy transfer in isolated LHC II studied by femtosecond pump-probe technique

CERN Document Server

Yang Yi; Liu Yuan; Liu Wei Min; Zhu Rong Yi; Qian Shi Xiong; Xu Chun He

2003-01-01

Excitation energy transfer in the isolated light-harvesting chlorophyll (Chl)-a/b protein complex of photosystem II (LHC II) was studied by the one-colour pump-probe technique with femtosecond time resolution. After exciting Chl-b by 638nm beam, the dynamic behaviour shows that the ultrafast energy transfer from Chl-b at positions of B2, B3, and B5 to the corresponding Chl-a molecules in monomeric subunit of LHC II is in the time scale of 230fs. While with the excitation of Chl-a at 678nm, the energy transfer between excitons of Chl-a molecules has the lifetime of about 370 fs, and two other slow decay components are due to the energy transfer between different Chl-a molecules in a monomeric subunit of LHC II or in different subunits, or due to change of molecular conformation. (20 refs).

Ultrafast Single and Multiexciton Energy Transfer in Semiconductor Nanoplatelets

Science.gov (United States)

Schaller, Richard

Photophysical processes such as fluorescence resonance energy transfer (FRET) enable optical antennas, wavelength down-conversion in light-emitting diodes (LEDs), and optical bio-sensing schemes. The rate and efficiency of this donor to acceptor transfer of excitation between chromophores dictates the utility of FRET and can unlock new device operation motifs including quantum-funnel solar cells and reduced gain thresholds. However, the fastest reported FRET time constants involving spherical quantum dots (QDs) (0.12-1 ns), do not outpace biexciton Auger recombination (0.01-0.1 ns), which impedes multiexciton-driven applications including electrically-pumped lasers and carrier-multiplication-enhanced photovoltaics. Precisely controlled, few-monolayer thick semiconductor nano-platelets with tens-of-nanometer diameters exhibit intense optical transitions and hundreds-of-picosecond Auger recombination, but heretofore lack FRET characterizations. We examine binary CdSe NPL solids and show that inter-plate FRET (~6-23 ps, presumably for co-facial arrangements) can occur 15-50 times faster than Auger recombination and demonstrate multiexcitonic FRET, making such materials ideal candidates for advanced technologies. This work was performed at the Center for Nanoscale Materials, a U.S. Department of Energy Office of Science User Facility under Contract No. DE-AC02-06CH11357.

Ultrafast energy transfer in dansylated POPAM--eosin complexes

Science.gov (United States)

Aumanen, Jukka; Lehtovuori, Viivi; Werner, Nicole; Richardt, Gabriele; van Heyst, Jeroen; Vögtle, Fritz; Korppi-Tommola, Jouko

2006-12-01

Excitation energy transfer (EET) in dendritic host-guest complexes has been studied. Three generations G2, G3 and G4 of dansyl substituted poly(propyleneamine) dendrimers (POPAM) were complexed with a fluorescent dye eosin in chloroform solution. Arrival of excitation from dansyls to eosin was monitored by femtosecond transient absorption spectroscopy. EET rates from the dansyls to eosin(s) are characterised by two time constants 1 ps and 6 ps independent of dendrimer generation. Relaxation processes in eosin were clearly faster when complexed with dendrimer than in solution. As several eosins are bound to G3 and G4 dendrimers, besides host-guest interaction, also eosin-eosin interactions may contribute to the faster relaxation observed in these complexes.

The effect of solvent relaxation time constants on free energy gap law for ultrafast charge recombination following photoinduced charge separation.

Science.gov (United States)

Mikhailova, Valentina A; Malykhin, Roman E; Ivanov, Anatoly I

2018-05-16

To elucidate the regularities inherent in the kinetics of ultrafast charge recombination following photoinduced charge separation in donor-acceptor dyads in solutions, the simulations of the kinetics have been performed within the stochastic multichannel point-transition model. Increasing the solvent relaxation time scales has been shown to strongly vary the dependence of the charge recombination rate constant on the free energy gap. In slow relaxing solvents the non-equilibrium charge recombination occurring in parallel with solvent relaxation is very effective so that the charge recombination terminates at the non-equilibrium stage. This results in a crucial difference between the free energy gap laws for the ultrafast charge recombination and the thermal charge transfer. For the thermal reactions the well-known Marcus bell-shaped dependence of the rate constant on the free energy gap is realized while for the ultrafast charge recombination only a descending branch is predicted in the whole area of the free energy gap exceeding 0.2 eV. From the available experimental data on the population kinetics of the second and first excited states for a series of Zn-porphyrin-imide dyads in toluene and tetrahydrofuran solutions, an effective rate constant of the charge recombination into the first excited state has been calculated. The obtained rate constant being very high is nearly invariable in the area of the charge recombination free energy gap from 0.2 to 0.6 eV that supports the theoretical prediction.

Ultrafast coherence transfer in DNA-templated silver nanoclusters

DEFF Research Database (Denmark)

Thyrhaug, Erling; Bogh, Sidsel Ammitzbøll; Carro, Miguel

2017-01-01

DNA-templated silver nanoclusters of a few tens of atoms or less have come into prominence over the last several years due to very strong absorption and efficient emission. Applications in microscopy and sensing have already been realized, however little is known about the excited-state structure...... and dynamics in these clusters. Here we report on a multidimensional spectroscopy investigation of the energy-level structure and the early-time relaxation cascade, which eventually results in the population of an emitting state. We find that the ultrafast intramolecular relaxation is strongly coupled...

Quantum modeling of ultrafast photoinduced charge separation

Science.gov (United States)

Rozzi, Carlo Andrea; Troiani, Filippo; Tavernelli, Ivano

2018-01-01

Phenomena involving electron transfer are ubiquitous in nature, photosynthesis and enzymes or protein activity being prominent examples. Their deep understanding thus represents a mandatory scientific goal. Moreover, controlling the separation of photogenerated charges is a crucial prerequisite in many applicative contexts, including quantum electronics, photo-electrochemical water splitting, photocatalytic dye degradation, and energy conversion. In particular, photoinduced charge separation is the pivotal step driving the storage of sun light into electrical or chemical energy. If properly mastered, these processes may also allow us to achieve a better command of information storage at the nanoscale, as required for the development of molecular electronics, optical switching, or quantum technologies, amongst others. In this Topical Review we survey recent progress in the understanding of ultrafast charge separation from photoexcited states. We report the state-of-the-art of the observation and theoretical description of charge separation phenomena in the ultrafast regime mainly focusing on molecular- and nano-sized solar energy conversion systems. In particular, we examine different proposed mechanisms driving ultrafast charge dynamics, with particular regard to the role of quantum coherence and electron-nuclear coupling, and link experimental observations to theoretical approaches based either on model Hamiltonians or on first principles simulations.

Direct determination of resonance energy transfer in photolyase: structural alignment for the functional state.

Science.gov (United States)

Tan, Chuang; Guo, Lijun; Ai, Yuejie; Li, Jiang; Wang, Lijuan; Sancar, Aziz; Luo, Yi; Zhong, Dongping

2014-11-13

Photoantenna is essential to energy transduction in photoinduced biological machinery. A photoenzyme, photolyase, has a light-harvesting pigment of methenyltetrahydrofolate (MTHF) that transfers its excitation energy to the catalytic flavin cofactor FADH¯ to enhance DNA-repair efficiency. Here we report our systematic characterization and direct determination of the ultrafast dynamics of resonance energy transfer from excited MTHF to three flavin redox states in E. coli photolyase by capturing the intermediates formed through the energy transfer and thus excluding the electron-transfer quenching pathway. We observed 170 ps for excitation energy transferring to the fully reduced hydroquinone FADH¯, 20 ps to the fully oxidized FAD, and 18 ps to the neutral semiquinone FADH(•), and the corresponding orientation factors (κ(2)) were determined to be 2.84, 1.53 and 1.26, respectively, perfectly matching with our calculated theoretical values. Thus, under physiological conditions and over the course of evolution, photolyase has adopted the optimized orientation of its photopigment to efficiently convert solar energy for repair of damaged DNA.

Vibrational energy on surfaces: Ultrafast flash-thermal conductance of molecular monolayers

Science.gov (United States)

Dlott, Dana

2008-03-01

Vibrational energy flow through molecules remains a perennial problem in chemical physics. Usually vibrational energy dynamics are viewed through the lens of time-dependent level populations. This is natural because lasers naturally pump and probe vibrational transitions, but it is also useful to think of vibrational energy as being conducted from one location in a molecule to another. We have developed a new technique where energy is driven into a specific part of molecules adsorbed on a metal surface, and ultrafast nonlinear coherent vibrational spectroscopy is used to watch the energy arrive at another part. This technique is the analog of a flash thermal conductance apparatus, except it probes energy flow with angstrom spatial and femtosecond temporal resolution. Specific examples to be presented include energy flow along alkane chains, and energy flow into substituted benzenes. Ref: Z. Wang, J. A. Carter, A. Lagutchev, Y. K. Koh, N.-H. Seong, D. G. Cahill, and D. D. Dlott, Ultrafast flash thermal conductance of molecular chains, Science 317, 787-790 (2007). This material is based upon work supported by the National Science Foundation under award DMR 0504038 and the Air Force Office of Scientific Research under award FA9550-06-1-0235.

Adlayer structure dependent ultrafast desorption dynamics in carbon monoxide adsorbed on Pd (111)

Energy Technology Data Exchange (ETDEWEB)

Hong, Sung-Young; Camillone, Nina R.; Camillone, Nicholas, E-mail: nicholas@bnl.gov [Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973 (United States); Xu, Pan [Department of Chemistry, Stony Brook University, Stony Brook, New York 11794 (United States); White, Michael G. [Chemistry Department, Brookhaven National Laboratory, Upton, New York 11973 (United States); Department of Chemistry, Stony Brook University, Stony Brook, New York 11794 (United States)

2016-07-07

We report our ultrafast photoinduced desorption investigation of the coverage dependence of substrate–adsorbate energy transfer in carbon monoxide adlayers on the (111) surface of palladium. As the CO coverage is increased, the adsorption site population shifts from all threefold hollows (up to 0.33 ML), to bridge and near bridge (>0.5 to 0.6 ML) and finally to mixed threefold hollow plus top site (at saturation at 0.75 ML). We show that between 0.24 and 0.75 ML this progression of binding site motifs is accompanied by two remarkable features in the ultrafast photoinduced desorption of the adsorbates: (i) the desorption probability increases roughly two orders magnitude, and (ii) the adsorbate–substrate energy transfer rate observed in two-pulse correlation experiments varies nonmonotonically, having a minimum at intermediate coverages. Simulations using a phenomenological model to describe the adsorbate–substrate energy transfer in terms of frictional coupling indicate that these features are consistent with an adsorption-site dependent electron-mediated energy coupling strength, η{sub el}, that decreases with binding site in the order: three-fold hollow > bridge and near bridge > top site. This weakening of η{sub el} largely counterbalances the decrease in the desorption activation energy that accompanies this progression of adsorption site motifs, moderating what would otherwise be a rise of several orders of magnitude in the desorption probability. Within this framework, the observed energy transfer rate enhancement at saturation coverage is due to interadsorbate energy transfer from the copopulation of molecules bound in three-fold hollows to their top-site neighbors.

Hotspot-mediated non-dissipative and ultrafast plasmon passage

Science.gov (United States)

Roller, Eva-Maria; Besteiro, Lucas V.; Pupp, Claudia; Khorashad, Larousse Khosravi; Govorov, Alexander O.; Liedl, Tim

2017-08-01

Plasmonic nanoparticles hold great promise as photon handling elements and as channels for coherent transfer of energy and information in future all-optical computing devices. Coherent energy oscillations between two spatially separated plasmonic entities via a virtual middle state exemplify electron-based population transfer, but their realization requires precise nanoscale positioning of heterogeneous particles. Here, we show the assembly and optical analysis of a triple-particle system consisting of two gold nanoparticles with an inter-spaced silver island. We observe strong plasmonic coupling between the spatially separated gold particles, mediated by the connecting silver particle, with almost no dissipation of energy. As the excitation energy of the silver island exceeds that of the gold particles, only quasi-occupation of the silver transfer channel is possible. We describe this effect both with exact classical electrodynamic modelling and qualitative quantum-mechanical calculations. We identify the formation of strong hotspots between all particles as the main mechanism for the lossless coupling and thus coherent ultrafast energy transfer between the remote partners. Our findings could prove useful for quantum gate operations, as well as for classical charge and information transfer processes.

Decay time shortening of fluorescence from donor-acceptor pair proteins using ultrafast time-resolved fluorescence resonance energy transfer spectroscopy

International Nuclear Information System (INIS)

Baba, Motoyoshi; Suzuki, Masayuki; Ganeev, Rashid A.; Kuroda, Hiroto; Ozaki, Tsuneyuki; Hamakubo, Takao; Masuda, Kazuyuki; Hayashi, Masahiro; Sakihama, Toshiko; Kodama, Tatsuhiko; Kozasa, Tohru

2007-01-01

We improved an ultrafast time-resolved fluorescence resonance energy transfer (FRET) spectroscopy system and measured directly the decrease in the fluorescence decay time of the FRET signal, without any entanglement of components in the picosecond time scale from the donor-acceptor protein pairs (such as cameleon protein for calcium ion indicator, and ligand-activated GRIN-Go proteins pair). The drastic decrease in lifetime of the donor protein fluorescence under the FRET condition (e.g. a 47.8% decrease for a GRIN-Go protein pair) proves the deformation dynamics between donor and acceptor fluorescent proteins in an activated state of a mixed donor-acceptor protein pair. This study is the first clear evidence of physical contact of the GRIN-Go proteins pair using time-resolved FRET system. G protein-coupled receptors (GPCRs) are the most important protein family for the recognition of many chemical substances at the cell surface. They are the targets of many drugs. Simultaneously, we were able to observe the time-resolved spectra of luminous proteins at the initial stage under the FRET condition, within 10 ns from excitation. This new FRET system allows us to trace the dynamics of the interaction between proteins at the ligand-induced activated state, molecular structure change and combination or dissociation. It will be a key technology for the development of protein chip technology

Ultrafast Excited-State Dynamics of Diketopyrrolopyrrole (DPP)-Based Materials: Static versus Diffusion-Controlled Electron Transfer Process

KAUST Repository

Alsulami, Qana

2015-06-25

Singlet-to-triplet intersystem crossing (ISC) and photoinduced electron transfer (PET) of platinum(II) containing diketopyrrolopyrrole (DPP) oligomer in the absence and presence of strong electron-acceptor tetracyanoethylene (TCNE) were investigated using femtosecond and nanosecond transient absorption spectroscopy with broadband capabilities. The role of platinum(II) incorporation in those photophysical properties was evaluated by comparing the excited-state dynamics of DPP with and without the metal centers. The steady-state measurements reveal that platinum(II) incorporation facilitates dramatically the interactions between DPP-Pt(acac) and TCNE, resulting in charge transfer (CT) complex formation. The transient absorption spectra in the absence of TCNE reveal ultrafast ISC of DPP-Pt(acac) followed by their long-lived triplet state. In the presence of TCNE, PET from the excited DPP-Pt(acac) and DPP to TCNE, forming the radical ion pairs. The ultrafast PET which occurs statically from DPP-Pt(acac) to TCNE in picosecond regime, is much faster than that from DPP to TCNE (nanosecond time scale) which is diffusion-controlled process, providing clear evidence that PET rate is eventually controlled by the platinum(II) incorporation.

Ultrafast Excited-State Dynamics of Diketopyrrolopyrrole (DPP)-Based Materials: Static versus Diffusion-Controlled Electron Transfer Process

KAUST Repository

Alsulami, Qana; Aly, Shawkat Mohammede; Goswami, Subhadip; Alarousu, Erkki; Usman, Anwar; Schanze, Kirk S.; Mohammed, Omar F.

2015-01-01

Singlet-to-triplet intersystem crossing (ISC) and photoinduced electron transfer (PET) of platinum(II) containing diketopyrrolopyrrole (DPP) oligomer in the absence and presence of strong electron-acceptor tetracyanoethylene (TCNE) were investigated using femtosecond and nanosecond transient absorption spectroscopy with broadband capabilities. The role of platinum(II) incorporation in those photophysical properties was evaluated by comparing the excited-state dynamics of DPP with and without the metal centers. The steady-state measurements reveal that platinum(II) incorporation facilitates dramatically the interactions between DPP-Pt(acac) and TCNE, resulting in charge transfer (CT) complex formation. The transient absorption spectra in the absence of TCNE reveal ultrafast ISC of DPP-Pt(acac) followed by their long-lived triplet state. In the presence of TCNE, PET from the excited DPP-Pt(acac) and DPP to TCNE, forming the radical ion pairs. The ultrafast PET which occurs statically from DPP-Pt(acac) to TCNE in picosecond regime, is much faster than that from DPP to TCNE (nanosecond time scale) which is diffusion-controlled process, providing clear evidence that PET rate is eventually controlled by the platinum(II) incorporation.

Electrically-driven GHz range ultrafast graphene light emitter (Conference Presentation)

Science.gov (United States)

Kim, Youngduck; Gao, Yuanda; Shiue, Ren-Jye; Wang, Lei; Aslan, Ozgur Burak; Kim, Hyungsik; Nemilentsau, Andrei M.; Low, Tony; Taniguchi, Takashi; Watanabe, Kenji; Bae, Myung-Ho; Heinz, Tony F.; Englund, Dirk R.; Hone, James

2017-02-01

Ultrafast electrically driven light emitter is a critical component in the development of the high bandwidth free-space and on-chip optical communications. Traditional semiconductor based light sources for integration to photonic platform have therefore been heavily studied over the past decades. However, there are still challenges such as absence of monolithic on-chip light sources with high bandwidth density, large-scale integration, low-cost, small foot print, and complementary metal-oxide-semiconductor (CMOS) technology compatibility. Here, we demonstrate the first electrically driven ultrafast graphene light emitter that operate up to 10 GHz bandwidth and broadband range (400 1600 nm), which are possible due to the strong coupling of charge carriers in graphene and surface optical phonons in hBN allow the ultrafast energy and heat transfer. In addition, incorporation of atomically thin hexagonal boron nitride (hBN) encapsulation layers enable the stable and practical high performance even under the ambient condition. Therefore, electrically driven ultrafast graphene light emitters paves the way towards the realization of ultrahigh bandwidth density photonic integrated circuits and efficient optical communications networks.

Imaging the Ultrafast Photoelectron Transfer Process in Alizarin-TiO2

Directory of Open Access Journals (Sweden)

Tatiana Gomez

2015-07-01

Full Text Available In this work, we adopt a quantum mechanical approach based on time-dependent density functional theory (TDDFT to study the optical and electronic properties of alizarin supported on TiO2 nano-crystallites, as a prototypical dye-sensitized solar cell. To ensure proper alignment of the donor (alizarin and acceptor (TiO2 nano-crystallite levels, static optical excitation spectra are simulated using time-dependent density functional theory in response. The ultrafast photoelectron transfer from the dye to the cluster is simulated using an explicitly time-dependent, one-electron TDDFT ansatz. The model considers the δ-pulse excitation of a single active electron localized in the dye to the complete set of energetically accessible, delocalized molecular orbitals of the dye/nano-crystallite complex. A set of quantum mechanical tools derived from the transition electronic flux density is introduced to visualize and analyze the process in real time. The evolution of the created wave packet subject to absorbing boundary conditions at the borders of the cluster reveal that, while the electrons of the aromatic rings of alizarin are heavily involved in an ultrafast charge redistribution between the carbonyl groups of the dye molecule, they do not contribute positively to the electron injection and, overall, they delay the process.

Ultrafast Dynamics of Dansylated POPAM Dendrimers and Energy Transfer in their Dye Complexes

Science.gov (United States)

Aumanen, J.; Kesti, T.; Sundström, V.; Vögtle, F.; Korppi-Tommola, J.

We have studied internal dynamics of dansylated poly(propyleneamine) dendrimers of different generations in solution and excitation energy transfer from dansyl chromophores to xanthene dyes that form van der Waals complexes with the dendrimers

Ultrafast excited state processes in Roseobacter denitrificans antennae: comparison of isolated complexes and native membranes

NARCIS (Netherlands)

Ferretti, M.; Duquesne, K.; Sturgis, J.N.; van Grondelle, R.

2014-01-01

Roseobacter (Rsb.) denitrificans is a marine aerobic anoxygenic photosynthetic purple bacterium with an unusually high-800 nm absorption band. Ultrafast excited state processes have been intensively studied in the past in order to understand why the energy transfer efficiency between photosynthetic

Ultrafast static and diffusion-controlled electron transfer at Ag 29 nanocluster/molecular acceptor interfaces

KAUST Repository

Aly, Shawkat Mohammede; AbdulHalim, Lina G.; Besong, Tabot M.D.; Soldan, Giada; Bakr, Osman; Mohammed, Omar F.

2015-01-01

Efficient absorption of visible light and a long-lived excited state lifetime of silver nanoclusters (Ag29 NCs) are integral properties for these new clusters to serve as light-harvesting materials. Upon optical excitation, electron injection at Ag29 NC/methyl viologen (MV2+) interfaces is very efficient and ultrafast. Interestingly, our femto- and nanosecond time-resolved results demonstrate clearly that both dynamic and static electron transfer mechanisms are involved in photoluminescence quenching of Ag29 NCs. © 2016 The Royal Society of Chemistry.

Ultrafast static and diffusion-controlled electron transfer at Ag 29 nanocluster/molecular acceptor interfaces

KAUST Repository

Aly, Shawkat Mohammede

2015-10-29

Efficient absorption of visible light and a long-lived excited state lifetime of silver nanoclusters (Ag29 NCs) are integral properties for these new clusters to serve as light-harvesting materials. Upon optical excitation, electron injection at Ag29 NC/methyl viologen (MV2+) interfaces is very efficient and ultrafast. Interestingly, our femto- and nanosecond time-resolved results demonstrate clearly that both dynamic and static electron transfer mechanisms are involved in photoluminescence quenching of Ag29 NCs. © 2016 The Royal Society of Chemistry.

Determination of hot carrier energy distributions from inversion of ultrafast pump-probe reflectivity measurements.

Science.gov (United States)

Heilpern, Tal; Manjare, Manoj; Govorov, Alexander O; Wiederrecht, Gary P; Gray, Stephen K; Harutyunyan, Hayk

2018-05-10

Developing a fundamental understanding of ultrafast non-thermal processes in metallic nanosystems will lead to applications in photodetection, photochemistry and photonic circuitry. Typically, non-thermal and thermal carrier populations in plasmonic systems are inferred either by making assumptions about the functional form of the initial energy distribution or using indirect sensors like localized plasmon frequency shifts. Here we directly determine non-thermal and thermal distributions and dynamics in thin films by applying a double inversion procedure to optical pump-probe data that relates the reflectivity changes around Fermi energy to the changes in the dielectric function and in the single-electron energy band occupancies. When applied to normal incidence measurements our method uncovers the ultrafast excitation of a non-Fermi-Dirac distribution and its subsequent thermalization dynamics. Furthermore, when applied to the Kretschmann configuration, we show that the excitation of propagating plasmons leads to a broader energy distribution of electrons due to the enhanced Landau damping.

Ultrafast Librational Relaxation of H2O in Liquid Water

DEFF Research Database (Denmark)

Petersen, Jakob; Møller, Klaus Braagaard; Rey, Rossend

2013-01-01

The ultrafast librational (hindered rotational) relaxation of a rotationally excited H2O molecule in pure liquid water is investigated by means of classical nonequilibrium molecular dynamics simulations and a power and work analysis. This analysis allows the mechanism of the energy transfer from...... the excited H2O to its water neighbors, which occurs on a sub-100 fs time scale, to be followed in molecular detail, i.e., to determine which water molecules receive the energy and in which degrees of freedom. It is found that the dominant energy flow is to the four hydrogen-bonded water partners in the first...

Spectral heterogeneity and carotenoid-to-bacteriochlorophyll energy transfer in LH2 light-harvesting complexes from Allochromatium vinosum.

Science.gov (United States)

Magdaong, Nikki M; LaFountain, Amy M; Hacking, Kirsty; Niedzwiedzki, Dariusz M; Gibson, George N; Cogdell, Richard J; Frank, Harry A

2016-02-01

Photosynthetic organisms produce a vast array of spectral forms of antenna pigment-protein complexes to harvest solar energy and also to adapt to growth under the variable environmental conditions of light intensity, temperature, and nutrient availability. This behavior is exemplified by Allochromatium (Alc.) vinosum, a photosynthetic purple sulfur bacterium that produces different types of LH2 light-harvesting complexes in response to variations in growth conditions. In the present work, three different spectral forms of LH2 from Alc. vinosum, B800-820, B800-840, and B800-850, were isolated, purified, and examined using steady-state absorption and fluorescence spectroscopy, and ultrafast time-resolved absorption spectroscopy. The pigment composition of the LH2 complexes was analyzed by high-performance liquid chromatography, and all were found to contain five carotenoids: lycopene, anhydrorhodovibrin, spirilloxanthin, rhodopin, and rhodovibrin. Spectral reconstructions of the absorption and fluorescence excitation spectra based on the pigment composition revealed significantly more spectral heterogeneity in these systems compared to LH2 complexes isolated from other species of purple bacteria. The data also revealed the individual carotenoid-to-bacteriochlorophyll energy transfer efficiencies which were correlated with the kinetic data from the ultrafast transient absorption spectroscopic experiments. This series of LH2 complexes allows a systematic exploration of the factors that determine the spectral properties of the bound pigments and control the rate and efficiency of carotenoid-to-bacteriochlorophyll energy transfer.

Electron energy transfer effect in Au NS/CH3NH3PbI3-xClx heterostructures via localized surface plasmon resonance coupling.

Science.gov (United States)

Cai, Chunfeng; Zhai, Jizhi; Bi, Gang; Wu, Huizhen

2016-09-15

Localized surface plasmon resonance coupling effects (LSPR) have attracted much attention due to their interesting properties. This Letter demonstrates significant photoluminescence (PL) enhancement in the Au NS/CH3NH3PbI3-xClx heterostructures via the LSPR coupling. The observed PL emission enhancement is mainly attributed to the hot electron energy transfer effect related to the LSPR coupling. For the energy transfer effect, photo-generated electrons will be directly extracted into Au SPs, rather than relaxed into exciton states. This energy transfer process is much faster than the diffusion and relaxation time of free electrons, and may provide new ideas on the design of high-efficiency solar cells and ultrafast response photodetectors.

Effect of donor orientation on ultrafast intermolecular electron transfer in coumarin-amine systems

International Nuclear Information System (INIS)

Singh, P. K.; Nath, S.; Bhasikuttan, A. C.; Kumbhakar, M.; Mohanty, J.; Sarkar, S. K.; Mukherjee, T.; Pal, H.

2008-01-01

Effect of donor amine orientation on nondiffusive ultrafast intermolecular electron transfer (ET) reactions in coumarin-amine systems has been investigated using femtosecond fluorescence upconversion measurements. Intermolecular ET from different aromatic and aliphatic amines used as donor solvents to the excited coumarin-151 (C151) acceptor occurs with ultrafast rates such that the shortest fluorescence lifetime component (τ 1 ) is the measure of the fastest ET rate (τ 1 =τ ET fast =(k ET fast ) -1 ), assigned to the C151-amine contact pairs in which amine donors are properly oriented with respect to C151 to maximize the acceptor-donor electronic coupling (V el ). It is interestingly observed that as the amine solvents are diluted by suitable diluents (either keeping solvent dielectric constant similar or with increasing dielectric constant), the τ 1 remains almost in the similar range as long as the amine dilution does not cross a certain critical limit, which in terms of the amine mole fraction (x A ) is found to be ∼0.4 for aromatic amines and ∼0.8 for aliphatic amines. Beyond these dilutions in the two respective cases of the amine systems, the τ 1 values are seen to increase very sharply. The large difference in the critical x A values involving aromatic and aliphatic amine donors has been rationalized in terms of the largely different orientational restrictions for the ET reactions as imposed by the aliphatic (n-type) and aromatic (π-type) nature of the amine donors [A. K. Satpati et al., J. Mol. Struct. 878, 84 (2008)]. Since the highest occupied molecular orbital (HOMO) of the n-type aliphatic amines is mostly centralized at the amino nitrogen, only some specific orientations of these amines with respect to the close-contact acceptor dye [also of π-character; A. K. Satpati et al., J. Mol. Struct. 878, 84 (2008) and E. W. Castner et al., J. Phys. Chem. A 104, 2869 (2000)] can give suitable V el and thus ultrafast ET reaction. In contrary, the

Synchronous Measurement of Ultrafast Anisotropy Decay of the B850 in Bacterial LH2 Complex

International Nuclear Information System (INIS)

Wang Yun-Peng; Du Lu-Chao; Zhu Gang-Bei; Wang Zhuan; Weng Yu-Xiang

2015-01-01

Ultrafast anisotropic decay is a prominent parameter revealing ultrafast energy and electron transfer; however, it is difficult to be determined reliably owing to the requirement of a simultaneous availability of the parallel and perpendicular polarized decay kinetics. Nowadays, any measurement of anisotropic decay is a kind of approach to the exact simultaneity. Here we report a novel method for a synchronous ultrafast anisotropy decay measurement, which can well determine the anisotropy, even at a very early time, as the rising phase of the excitation laser pulse. The anisotropic decay of the B850 in bacterial light harvesting antenna complex LH2 of Rhodobacter sphaeroides in solution at room temperature with coherent excitation is detected by this method, which shows a polarization response time of 30 fs, and the energy transfer from the initial excitation to the bacteriochlorophylls in B850 ring takes about 70 fs. The anisotropic decay that is probed at the red side of the absorption spectrum, such as 880 nm, has an initial value of 0.4, corresponding to simulated emission, while the blue side with an anisotropy of 0.1 contributes to the ground-state bleaching. Our results show that the coherent excitation covering the whole ring might not be realized owing to the symmetry breaking of LH2: from C_9 symmetry in membrane to C_2 symmetry in solution. (atomic and molecular physics)

Synchronous Measurement of Ultrafast Anisotropy Decay of the B850 in Bacterial LH2 Complex

Science.gov (United States)

Wang, Yun-Peng; Du, Lu-Chao; Zhu, Gang-Bei; Wang, Zhuan; Weng, Yu-Xiang

2015-02-01

Ultrafast anisotropic decay is a prominent parameter revealing ultrafast energy and electron transfer; however, it is difficult to be determined reliably owing to the requirement of a simultaneous availability of the parallel and perpendicular polarized decay kinetics. Nowadays, any measurement of anisotropic decay is a kind of approach to the exact simultaneity. Here we report a novel method for a synchronous ultrafast anisotropy decay measurement, which can well determine the anisotropy, even at a very early time, as the rising phase of the excitation laser pulse. The anisotropic decay of the B850 in bacterial light harvesting antenna complex LH2 of Rhodobacter sphaeroides in solution at room temperature with coherent excitation is detected by this method, which shows a polarization response time of 30 fs, and the energy transfer from the initial excitation to the bacteriochlorophylls in B850 ring takes about 70 fs. The anisotropic decay that is probed at the red side of the absorption spectrum, such as 880 nm, has an initial value of 0.4, corresponding to simulated emission, while the blue side with an anisotropy of 0.1 contributes to the ground-state bleaching. Our results show that the coherent excitation covering the whole ring might not be realized owing to the symmetry breaking of LH2: from C9 symmetry in membrane to C2 symmetry in solution.

Picosecond excitation energy transfer of allophycocyanin studied in solution and in crystals.

Science.gov (United States)

Ranjbar Choubeh, Reza; Sonani, Ravi R; Madamwar, Datta; Struik, Paul C; Bader, Arjen N; Robert, Bruno; van Amerongen, Herbert

2018-03-01

Cyanobacteria perform photosynthesis with the use of large light-harvesting antennae called phycobilisomes (PBSs). These hemispherical PBSs contain hundreds of open-chain tetrapyrrole chromophores bound to different peptides, providing an arrangement in which excitation energy is funnelled towards the PBS core from where it can be transferred to photosystem I and/or photosystem II. In the PBS core, many allophycocyanin (APC) trimers are present, red-light-absorbing phycobiliproteins that covalently bind phycocyanobilin (PCB) chromophores. APC trimers were amongst the first light-harvesting complexes to be crystallized. APC trimers have two spectrally different PCBs per monomer, a high- and a low-energy pigment. The crystal structure of the APC trimer reveals the close distance (~21 Å) between those two chromophores (the distance within one monomer is ~51 Å) and this explains the ultrafast (~1 ps) excitation energy transfer (EET) between them. Both chromophores adopt a somewhat different structure, which is held responsible for their spectral difference. Here we used spectrally resolved picosecond fluorescence to study EET in these APC trimers both in crystallized and in solubilized form. We found that not all closely spaced pigment couples consist of a low- and a high-energy pigment. In ~10% of the cases, a couple consists of two high-energy pigments. EET to a low-energy pigment, which can spectrally be resolved, occurs on a time scale of tens of picoseconds. This transfer turns out to be three times faster in the crystal than in the solution. The spectral characteristics and the time scale of this transfer component are similar to what have been observed in the whole cells of Synechocystis sp. PCC 6803, for which it was ascribed to EET from C-phycocyanin to APC. The present results thus demonstrate that part of this transfer should probably also be ascribed to EET within APC trimers.

Ultrafast Science Opportunities with Electron Microscopy

Energy Technology Data Exchange (ETDEWEB)

DURR, HERMANN; Wang, X.J., ed.

2016-04-28

X-rays and electrons are two of the most fundamental probes of matter. When the Linac Coherent Light Source (LCLS), the world’s first x-ray free electron laser, began operation in 2009, it transformed ultrafast science with the ability to generate laser-like x-ray pulses from the manipulation of relativistic electron beams. This document describes a similar future transformation. In Transmission Electron Microscopy, ultrafast relativistic (MeV energy) electron pulses can achieve unsurpassed spatial and temporal resolution. Ultrafast temporal resolution will be the next frontier in electron microscopy and can ideally complement ultrafast x-ray science done with free electron lasers. This document describes the Grand Challenge science opportunities in chemistry, material science, physics and biology that arise from an MeV ultrafast electron diffraction & microscopy facility, especially when coupled with linac-based intense THz and X-ray pump capabilities.

Polymer-Polymer Förster Resonance Energy Transfer Significantly Boosts the Power Conversion Efficiency of Bulk-Heterojunction Solar Cells.

Science.gov (United States)

Gupta, Vinay; Bharti, Vishal; Kumar, Mahesh; Chand, Suresh; Heeger, Alan J

2015-08-01

Optically resonant donor polymers can exploit a wider range of the solar spectrum effectively without a complicated tandem design in an organic solar cell. Ultrafast Förster resonance energy transfer (FRET) in a polymer-polymer system that significantly improves the power conversion efficiency in bulk heterojunction polymer solar cells from 6.8% to 8.9% is demonstrated, thus paving the way to achieving 15% efficient solar cells. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Unveiling the excited state energy transfer pathways in peridinin-chlorophyll a-protein by ultrafast multi-pulse transient absorption spectroscopy.

Science.gov (United States)

Redeckas, Kipras; Voiciuk, Vladislava; Zigmantas, Donatas; Hiller, Roger G; Vengris, Mikas

2017-04-01

Time-resolved multi-pulse methods were applied to investigate the excited state dynamics, the interstate couplings, and the excited state energy transfer pathways between the light-harvesting pigments in peridinin-chlorophyll a-protein (PCP). The utilized pump-dump-probe techniques are based on perturbation of the regular PCP energy transfer pathway. The PCP complexes were initially excited with an ultrashort pulse, resonant to the S 0 →S 2 transition of the carotenoid peridinin. A portion of the peridinin-based emissive intramolecular charge transfer (ICT) state was then depopulated by applying an ultrashort NIR pulse that perturbed the interaction between S 1 and ICT states and the energy flow from the carotenoids to the chlorophylls. The presented data indicate that the peridinin S 1 and ICT states are spectrally distinct and coexist in an excited state equilibrium in the PCP complex. Moreover, numeric analysis of the experimental data asserts ICT→Chl-a as the main energy transfer pathway in the photoexcited PCP systems. Copyright © 2017 Elsevier B.V. All rights reserved.

Ultrafast molecular dynamics illuminated with synchrotron radiation

International Nuclear Information System (INIS)

Bozek, John D.; Miron, Catalin

2015-01-01

Highlights: • Ultrafast molecular dynamics probed with synchrotron radiation. • Core-excitation as probe of ultrafast dynamics through core-hole lifetime. • Review of experimental and theoretical methods in ultrafast dynamics using core-level excitation. - Abstract: Synchrotron radiation is a powerful tool for studying molecular dynamics in small molecules in spite of the absence of natural matching between the X-ray pulse duration and the time scale of nuclear motion. Promoting core level electrons to unoccupied molecular orbitals simultaneously initiates two ultrafast processes, nuclear dynamics on the potential energy surfaces of the highly excited neutral intermediate state of the molecule on the one hand and an ultrafast electronic decay of the intermediate excited state to a cationic final state, characterized by a core hole lifetime. The similar time scales of these processes enable core excited pump-probe-type experiments to be performed with long duration X-ray pulses from a synchrotron source. Recent results obtained at the PLIEADES beamline concerning ultrafast dissociation of core excited states and molecular potential energy curve mapping facilitated by changes in the geometry of the short-lived intermediate core excited state are reviewed. High brightness X-ray beams combined with state-of-the art electron and ion-electron coincidence spectrometers and highly sophisticated theoretical methods are required to conduct these experiments and to achieve a full understanding of the experimental results.

Study of primary energy transfer process in ultrafast plastic scintillators

International Nuclear Information System (INIS)

Bengtson, B.; Moszynski, M.

1978-01-01

The study of the light-pulse shape, the initial delay of light pulses and the light yield of plastics prepared by a modification of the NE111 scintillator were performed. The NE111 scintillator doped with several quench agents, the plastics prepared as a solution of butyl PBD in PVT of different concentration and PVT alone were studied. The study confirmed that the light pulse shape from fast binary plastics is well described analytically by the convolution of the clipped Gaussian and exponential functions. The investigation of the PVT-butyl PBD plastics shows that even more than three times larger concentration of butyl PBD compared to that of PBD in the NE111 solution does not improve the rise of the light pulse. Thus the rise time seems to be not controlled by the intermolecular energy transfer process. Finally, the observed rise time of the light pulse from the PVT sample was also approximated well by the Gaussian function. Altogether it brought a strong support for the earlier hypothesis that the initial slow rise of light pulses from plastic scintillators may come from the deexcitation of several higher levels of the solvent molecules excited by nuclear particles. (Auth.)

Ultrafast carrier dynamics in bilayer graphene studied by broadband infrared pump-probe spectroscopy

Science.gov (United States)

Limmer, Thomas; da Como, Enrico; Niggebaum, Alexander; Feldmann, Jochen

2010-03-01

Recently, bilayer graphene gained a large interest because of its electrically tunable gap appearing in the middle infrared part of the electromagnetic spectrum. This feature is expected to open a number of applications of bilayer graphene in optoelectronics. In this communication we report on the first pump-probe experiment on a single bilayer flake with an unprecedented probe photon energy interval (0.25 -- 1.3 eV). Single flakes were prepared by mechanical exfoliation of graphite and transferred to calcium fluoride substrates. When illuminated with 800 nm (1.5 eV) pump pulses the induced change in transmission shows an ultrafast saturation of the interband transitions from 1.3 to 0.5 eV. In this energy range the saturation recovery occurs within 3 ps and is consistent with an ultrafast relaxation of hot carriers. Interestingly, we report on the observation of a resonance at 0.4 eV characterized by a longer dynamics. The results are discussed considering many-body interactions.

Solvent-assisted multistage nonequilibrium electron transfer in rigid supramolecular systems: Diabatic free energy surfaces and algorithms for numerical simulations

Science.gov (United States)

Feskov, Serguei V.; Ivanov, Anatoly I.

2018-03-01

An approach to the construction of diabatic free energy surfaces (FESs) for ultrafast electron transfer (ET) in a supramolecule with an arbitrary number of electron localization centers (redox sites) is developed, supposing that the reorganization energies for the charge transfers and shifts between all these centers are known. Dimensionality of the coordinate space required for the description of multistage ET in this supramolecular system is shown to be equal to N - 1, where N is the number of the molecular centers involved in the reaction. The proposed algorithm of FES construction employs metric properties of the coordinate space, namely, relation between the solvent reorganization energy and the distance between the two FES minima. In this space, the ET reaction coordinate zn n' associated with electron transfer between the nth and n'th centers is calculated through the projection to the direction, connecting the FES minima. The energy-gap reaction coordinates zn n' corresponding to different ET processes are not in general orthogonal so that ET between two molecular centers can create nonequilibrium distribution, not only along its own reaction coordinate but along other reaction coordinates too. This results in the influence of the preceding ET steps on the kinetics of the ensuing ET. It is important for the ensuing reaction to be ultrafast to proceed in parallel with relaxation along the ET reaction coordinates. Efficient algorithms for numerical simulation of multistage ET within the stochastic point-transition model are developed. The algorithms are based on the Brownian simulation technique with the recrossing-event detection procedure. The main advantages of the numerical method are (i) its computational complexity is linear with respect to the number of electronic states involved and (ii) calculations can be naturally parallelized up to the level of individual trajectories. The efficiency of the proposed approach is demonstrated for a model

Molecular-structure control of ultrafast electron injection at cationic porphyrin-CdTe quantum dot interfaces

KAUST Repository

Aly, Shawkat Mohammede

2015-03-05

Charge transfer (CT) at donor (D)/acceptor (A) interfaces is central to the functioning of photovoltaic and light-emitting devices. Understanding and controlling this process on the molecular level has been proven to be crucial for optimizing the performance of many energy-challenge relevant devices. Here, we report the experimental observations of controlled on/off ultrafast electron transfer (ET) at cationic porphyrin-CdTe quantum dot (QD) interfaces using femto- and nanosecond broad-band transient absorption (TA) spectroscopy. The time-resolved data demonstrate how one can turn on/off the electron injection from porphyrin to the CdTe QDs. With careful control of the molecular structure, we are able to tune the electron injection at the porphyrin-CdTe QD interface from zero to very efficient and ultrafast. In addition, our data demonstrate that the ET process occurs within our temporal resolution of 120 fs, which is one of the fastest times recorded for organic photovoltaics. © 2015 American Chemical Society.

Excited-state intramolecular proton transfer of 2-acetylindan-1,3-dione studied by ultrafast absorption and fluorescence spectroscopy

Directory of Open Access Journals (Sweden)

Pramod Kumar Verma

2016-03-01

Full Text Available We employ transient absorption from the deep-UV to the visible region and fluorescence upconversion to investigate the photoinduced excited-state intramolecular proton-transfer dynamics in a biologically relevant drug molecule, 2-acetylindan-1,3-dione. The molecule is a ß-diketone which in the electronic ground state exists as exocyclic enol with an intramolecular H-bond. Upon electronic excitation at 300 nm, the first excited state of the exocyclic enol is initially populated, followed by ultrafast proton transfer (≈160 fs to form the vibrationally hot endocyclic enol. Subsequently, solvent-induced vibrational relaxation takes place (≈10 ps followed by decay (≈390 ps to the corresponding ground state.

Photonic-assisted ultrafast THz wireless access

DEFF Research Database (Denmark)

Yu, Xianbin; Chen, Ying; Galili, Michael

THz technology has been considered feasible for ultrafast wireless data communi- cation, to meet the increasing demand on next-generation fast wireless access, e.g., huge data file transferring and fast mobile data stream access. This talk reviews recent progress in high-speed THz wireless...

Evidences from electron momentum spectroscopy for ultra-fast charge transfers and structural reorganizations in a floppy molecule: Ethanol

International Nuclear Information System (INIS)

Deleuze, Michael S; Hajgato, Balazs; Morini, Filippo

2009-01-01

Calculations of electron momentum distributions employing advanced Dyson orbital theories and statistical thermodynamics beyond the RRHO approximation fail to quantitatively reproduce the outermost momentum profile inferred from experiments on ethanol employing high resolution Electron Momentum Spectroscopy [1]. Study of the influence of nuclear dynamics in the initial ground state and final ionized state indicates that this discrepancy between theory and experiment reflects a charge transfer occurring during an ultra-fast dissociation of the ethanol radical cation into a methyl radical and H 2 C=O-H + .

Excited state electron and energy relays in supramolecular dinuclear complexes revealed by ultrafast optical and X-ray transient absorption spectroscopy.

Science.gov (United States)

Hayes, Dugan; Kohler, Lars; Hadt, Ryan G; Zhang, Xiaoyi; Liu, Cunming; Mulfort, Karen L; Chen, Lin X

2018-01-28

The kinetics of photoinduced electron and energy transfer in a family of tetrapyridophenazine-bridged heteroleptic homo- and heterodinuclear copper(i) bis(phenanthroline)/ruthenium(ii) polypyridyl complexes were studied using ultrafast optical and multi-edge X-ray transient absorption spectroscopies. This work combines the synthesis of heterodinuclear Cu(i)-Ru(ii) analogs of the homodinuclear Cu(i)-Cu(i) targets with spectroscopic analysis and electronic structure calculations to first disentangle the dynamics at individual metal sites by taking advantage of the element and site specificity of X-ray absorption and theoretical methods. The excited state dynamical models developed for the heterodinuclear complexes are then applied to model the more challenging homodinuclear complexes. These results suggest that both intermetallic charge and energy transfer can be observed in an asymmetric dinuclear copper complex in which the ground state redox potentials of the copper sites are offset by only 310 meV. We also demonstrate the ability of several of these complexes to effectively and unidirectionally shuttle energy between different metal centers, a property that could be of great use in the design of broadly absorbing and multifunctional multimetallic photocatalysts. This work provides an important step toward developing both a fundamental conceptual picture and a practical experimental handle with which synthetic chemists, spectroscopists, and theoreticians may collaborate to engineer cheap and efficient photocatalytic materials capable of performing coulombically demanding chemical transformations.

Highly efficient energy transfer from a carbonyl carotenoid to chlorophyll a in the main light harvesting complex of Chromera velia.

Science.gov (United States)

Durchan, Milan; Keşan, Gürkan; Slouf, Václav; Fuciman, Marcel; Staleva, Hristina; Tichý, Josef; Litvín, Radek; Bína, David; Vácha, František; Polívka, Tomáš

2014-10-01

We report on energy transfer pathways in the main light-harvesting complex of photosynthetic relative of apicomplexan parasites, Chromera velia. This complex, denoted CLH, belongs to the family of FCP proteins and contains chlorophyll (Chl) a, violaxanthin, and the so far unidentified carbonyl carotenoid related to isofucoxanthin. The overall carotenoid-to-Chl-a energy transfer exhibits efficiency over 90% which is the largest among the FCP-like proteins studied so far. Three spectroscopically different isofucoxanthin-like molecules were identified in CLH, each having slightly different energy transfer efficiency that increases from isofucoxanthin-like molecules absorbing in the blue part of the spectrum to those absorbing in the reddest part of spectrum. Part of the energy transfer from carotenoids proceeds via the ultrafast S2 channel of both the violaxanthin and isofucoxanthin-like carotenoid, but major energy transfer pathway proceeds via the S1/ICT state of the isofucoxanthin-like carotenoid. Two S1/ICT-mediated channels characterized by time constants of ~0.5 and ~4ps were found. For the isofucoxanthin-like carotenoid excited at 480nm the slower channel dominates, while those excited at 540nm employs predominantly the fast 0.5ps channel. Comparing these data with the excited-state properties of the isofucoxanthin-like carotenoid in solution we conclude that, contrary to other members of the FCP family employing carbonyl carotenoids, CLH complex suppresses the charge transfer character of the S1/ICT state of the isofucoxanthin-like carotenoid to achieve the high carotenoid-to-Chl-a energy transfer efficiency. Copyright © 2014 Elsevier B.V. All rights reserved.

Ultrafast proton shuttling in Psammocora cyan fluorescent protein.

Science.gov (United States)

Kennis, John T M; van Stokkum, Ivo H M; Peterson, Dayna S; Pandit, Anjali; Wachter, Rebekka M

2013-09-26

Cyan, green, yellow, and red fluorescent proteins (FPs) homologous to green fluorescent protein (GFP) are used extensively as model systems to study fundamental processes in photobiology, such as the capture of light energy by protein-embedded chromophores, color tuning by the protein matrix, energy conversion by Förster resonance energy transfer (FRET), and excited-state proton transfer (ESPT) reactions. Recently, a novel cyan fluorescent protein (CFP) termed psamFP488 was isolated from the genus Psammocora of reef building corals. Within the cyan color class, psamFP488 is unusual because it exhibits a significantly extended Stokes shift. Here, we applied ultrafast transient absorption and pump-dump-probe spectroscopy to investigate the mechanistic basis of psamFP488 fluorescence, complemented with fluorescence quantum yield and dynamic light scattering measurements. Transient absorption spectroscopy indicated that, upon excitation at 410 nm, the stimulated cyan emission rises in 170 fs. With pump-dump-probe spectroscopy, we observe a very short-lived (110 fs) ground-state intermediate that we assign to the deprotonated, anionic chromophore. In addition, a minor fraction (14%) decays with 3.5 ps to the ground state. Structural analysis of homologous proteins indicates that Glu-167 is likely positioned in sufficiently close vicinity to the chromophore to act as a proton acceptor. Our findings support a model where unusually fast ESPT from the neutral chromophore to Glu-167 with a time constant of 170 fs and resulting emission from the anionic chromophore forms the basis of the large psamFP488 Stokes shift. When dumped to the ground state, the proton on neutral Glu is very rapidly shuttled back to the anionic chromophore in 110 fs. Proton shuttling in excited and ground states is a factor of 20-4000 faster than in GFP, which probably results from a favorable hydrogen-bonding geometry between the chromophore phenolic oxygen and the glutamate acceptor, possibly

Dexter energy transfer pathways.

Science.gov (United States)

Skourtis, Spiros S; Liu, Chaoren; Antoniou, Panayiotis; Virshup, Aaron M; Beratan, David N

2016-07-19

Energy transfer with an associated spin change of the donor and acceptor, Dexter energy transfer, is critically important in solar energy harvesting assemblies, damage protection schemes of photobiology, and organometallic opto-electronic materials. Dexter transfer between chemically linked donors and acceptors is bridge mediated, presenting an enticing analogy with bridge-mediated electron and hole transfer. However, Dexter coupling pathways must convey both an electron and a hole from donor to acceptor, and this adds considerable richness to the mediation process. We dissect the bridge-mediated Dexter coupling mechanisms and formulate a theory for triplet energy transfer coupling pathways. Virtual donor-acceptor charge-transfer exciton intermediates dominate at shorter distances or higher tunneling energy gaps, whereas virtual intermediates with an electron and a hole both on the bridge (virtual bridge excitons) dominate for longer distances or lower energy gaps. The effects of virtual bridge excitons were neglected in earlier treatments. The two-particle pathway framework developed here shows how Dexter energy-transfer rates depend on donor, bridge, and acceptor energetics, as well as on orbital symmetry and quantum interference among pathways.

Probing ultrafast changes of spin and charge density profiles with resonant XUV magnetic reflectivity at the free-electron laser FERMI.

Science.gov (United States)

Gutt, C; Sant, T; Ksenzov, D; Capotondi, F; Pedersoli, E; Raimondi, L; Nikolov, I P; Kiskinova, M; Jaiswal, S; Jakob, G; Kläui, M; Zabel, H; Pietsch, U

2017-09-01

We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M 2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q -resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Q z , we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

Quantum confinement-tunable ultrafast charge transfer at the PbS quantum dot and phenyl-C61-butyric acid methyl ester interface

KAUST Repository

El-Ballouli, AlA'A O.; Alarousu, Erkki Antero; Bernardi, Marco; Aly, Shawkat Mohammede; Lagrow, Alec P.; Bakr, Osman; Mohammed, Omar F.

2014-01-01

Quantum dot (QD) solar cells have emerged as promising low-cost alternatives to existing photovoltaic technologies. Here, we investigate charge transfer and separation at PbS QDs and phenyl-C61-butyric acid methyl ester (PCBM) interfaces using a combination of femtosecond broadband transient absorption (TA) spectroscopy and steady-state photoluminescence quenching measurements. We analyzed ultrafast electron injection and charge separation at PbS QD/PCBM interfaces for four different QD sizes and as a function of PCBM concentration. The results reveal that the energy band alignment, tuned by the quantum size effect, is the key element for efficient electron injection and charge separation processes. More specifically, the steady-state and time-resolved data demonstrate that only small-sized PbS QDs with a bandgap larger than 1 eV can transfer electrons to PCBM upon light absorption. We show that these trends result from the formation of a type-II interface band alignment, as a consequence of the size distribution of the QDs. Transient absorption data indicate that electron injection from photoexcited PbS QDs to PCBM occurs within our temporal resolution of 120 fs for QDs with bandgaps that achieve type-II alignment, while virtually all signals observed in smaller bandgap QD samples result from large bandgap outliers in the size distribution. Taken together, our results clearly demonstrate that charge transfer rates at QD interfaces can be tuned by several orders of magnitude by engineering the QD size distribution. The work presented here will advance both the design and the understanding of QD interfaces for solar energy conversion. © 2014 American Chemical Society.

Quantum confinement-tunable ultrafast charge transfer at the PbS quantum dot and phenyl-C61-butyric acid methyl ester interface

KAUST Repository

El-Ballouli, AlA'A O.

2014-05-14

Quantum dot (QD) solar cells have emerged as promising low-cost alternatives to existing photovoltaic technologies. Here, we investigate charge transfer and separation at PbS QDs and phenyl-C61-butyric acid methyl ester (PCBM) interfaces using a combination of femtosecond broadband transient absorption (TA) spectroscopy and steady-state photoluminescence quenching measurements. We analyzed ultrafast electron injection and charge separation at PbS QD/PCBM interfaces for four different QD sizes and as a function of PCBM concentration. The results reveal that the energy band alignment, tuned by the quantum size effect, is the key element for efficient electron injection and charge separation processes. More specifically, the steady-state and time-resolved data demonstrate that only small-sized PbS QDs with a bandgap larger than 1 eV can transfer electrons to PCBM upon light absorption. We show that these trends result from the formation of a type-II interface band alignment, as a consequence of the size distribution of the QDs. Transient absorption data indicate that electron injection from photoexcited PbS QDs to PCBM occurs within our temporal resolution of 120 fs for QDs with bandgaps that achieve type-II alignment, while virtually all signals observed in smaller bandgap QD samples result from large bandgap outliers in the size distribution. Taken together, our results clearly demonstrate that charge transfer rates at QD interfaces can be tuned by several orders of magnitude by engineering the QD size distribution. The work presented here will advance both the design and the understanding of QD interfaces for solar energy conversion. © 2014 American Chemical Society.

Self-phase modulation enabled, wavelength-tunable ultrafast fiber laser sources: an energy scalable approach.

Science.gov (United States)

Liu, Wei; Li, Chen; Zhang, Zhigang; Kärtner, Franz X; Chang, Guoqing

2016-07-11

We propose and demonstrate a new approach to implement a wavelength-tunable ultrafast fiber laser source suitable for multiphoton microscopy. We employ fiber-optic nonlinearities to broaden a narrowband optical spectrum generated by an Yb-fiber laser system and then use optical bandpass filters to select the leftmost or rightmost spectral lobes from the broadened spectrum. Detailed numerical modeling shows that self-phase modulation dominates the spectral broadening, self-steepening tends to blue shift the broadened spectrum, and stimulated Raman scattering is minimal. We also find that optical wave breaking caused by fiber dispersion slows down the shift of the leftmost/rightmost spectral lobes and therefore limits the wavelength tuning range of the filtered spectra. We show both numerically and experimentally that shortening the fiber used for spectral broadening while increasing the input pulse energy can overcome this dispersion-induced limitation; as a result, the filtered spectral lobes have higher power, constituting a powerful and practical approach for energy scaling the resulting femtosecond sources. We use two commercially available photonic crystal fibers to verify the simulation results. More specific, use of 20-mm fiber NL-1050-ZERO-2 enables us to implement an Yb-fiber laser based ultrafast source, delivering femtosecond (70-120 fs) pulses tunable from 825 nm to 1210 nm with >1 nJ pulse energy.

A coherent modified Redfield theory for excitation energy transfer in molecular aggregates

Energy Technology Data Exchange (ETDEWEB)

Hwang-Fu, Yu-Hsien; Chen, Wei; Cheng, Yuan-Chung, E-mail: yuanchung@ntu.edu.tw

2015-02-02

Highlights: • A CMRT method for coherent energy transfer in molecular aggregates was developed. • Applicability of the method was verified in two-site systems with various parameters. • CMRT accurately describes population dynamics in the FMO-complex. • The method is accurate in a large parameter space and computationally efficient. - Abstract: Excitation energy transfer (EET) is crucial in photosynthetic light harvesting, and quantum coherence has been recently proven to be a ubiquitous phenomenon in photosynthetic EET. In this work, we derive a coherent modified Redfield theory (CMRT) that generalizes the modified Redfield theory to treat coherence dynamics. We apply the CMRT method to simulate the EET in a dimer system and compare the results with those obtained from numerically exact path integral calculations. The comparison shows that CMRT provides excellent computational efficiency and accuracy within a large EET parameter space. Furthermore, we simulate the EET dynamics in the FMO complex at 77 K using CMRT. The results show pronounced non-Markovian effects and long-lasting coherences in the ultrafast EET, in excellent agreement with calculations using the hierarchy equation of motion approach. In summary, we have successfully developed a simple yet powerful framework for coherent EET dynamics in photosynthetic systems and organic materials.

Exciplex formation in bimolecular photoinduced electron-transfer investigated by ultrafast time-resolved infrared spectroscopy.

Science.gov (United States)

Koch, Marius; Letrun, Romain; Vauthey, Eric

2014-03-12

The dynamics of bimolecular photoinduced electron-transfer reactions has been investigated with three donor/acceptor (D/A) pairs in tetrahydrofuran (THF) and acetonitrile (ACN) using a combination of ultrafast spectroscopic techniques, including time-resolved infrared absorption. For the D/A pairs with the highest driving force of electron transfer, all transient spectroscopic features can be unambiguously assigned to the excited reactant and the ionic products. For the pair with the lowest driving force, three additional transient infrared bands, more intense in THF than in ACN, with a time dependence that differs from those of the other bands are observed. From their frequency and solvent dependence, these bands can be assigned to an exciplex. Moreover, polarization-resolved measurements point to a relatively well-defined mutual orientation of the constituents and to a slower reorientational time compared to those of the individual reactants. Thanks to the minimal overlap of the infrared signature of all transient species in THF, a detailed reaction scheme including the relevant kinetic and thermodynamic parameters could be deduced for this pair. This analysis reveals that the formation and recombination of the ion pair occur almost exclusively via the exciplex.

Ultrafast photoelectron spectroscopy of small molecule organic films

Science.gov (United States)

Read, Kendall Laine

As research in the field of ultrafast optics has produced shorter and shorter pulses, at an ever-widening range of frequencies, ultrafast spectroscopy has grown correspondingly. In particular, ultrafast photoelectron spectroscopy allows direct observation of electrons in transient or excited states, regardless of the eventual relaxation mechanisms. High-harmonic conversion of 800nm, femtosecond, Ti:sapphire laser pulses allows excite/probe spectroscopy down into atomic core level states. To this end, an ultrafast, X-UV photoelectron spectroscopic system is described, including design considerations for the high-harmonic generation line, the time of flight detector, and the subsequent data collection electronics. Using a similar experimental setup, I have performed several ultrafast, photoelectron excited state decay studies at the IBM, T. J. Watson Research Center. All of the observed materials were electroluminescent thin film organics, which have applications as the emitter layer in organic light emitting devices. The specific materials discussed are: Alq, BAlq, DPVBi, and Alq doped with DCM or DMQA. Alq:DCM is also known to lase at low photoexcitation thresholds. A detailed understanding of the involved relaxation mechanisms is beneficial to both applications. Using 3.14 eV excite, and 26.7 eV probe, 90 fs laser pulses, we have observed the lowest unoccupied molecular orbital (LUMO) decay rate over the first 200 picoseconds. During this time, diffusion is insignificant, and all dynamics occur in the absence of electron transport. With excitation intensities in the range of 100μJ/cm2, we have modeled the Alq, BAlq, and DPVBi decays via bimolecular singlet-singlet annihilation. At similar excitations, we have modeled the Alq:DCM decay via Förster transfer, stimulated emission, and excimeric formation. Furthermore, the Alq:DCM occupied to unoccupied molecular orbital energy gap was seen to shrink as a function of excite-to-probe delay, in accordance with the

Ultrafast multi-pulse transient absorption spectroscopy of fucoxanthin chlorophyll a protein from Phaeodactylum tricornutum.

Science.gov (United States)

West, Robert G; Bína, David; Fuciman, Marcel; Kuznetsova, Valentyna; Litvín, Radek; Polívka, Tomáš

2018-05-01

We have applied femtosecond transient absorption spectroscopy in pump-probe and pump-dump-probe regimes to study energy transfer between fucoxanthin and Chl a in fucoxanthin-Chl a complex from the pennate diatom Phaeodactylum tricornutum. Experiments were carried out at room temperature and 77 K to reveal temperature dependence of energy transfer. At both temperatures, the ultrafast (pump-dump-probe regime, with the dump pulse centered in the spectral region of ICT stimulated emission at 950 nm and applied at 2 ps after excitation, proved that the S 1 and ICT states of fucoxanthin in FCP are individual, yet coupled entities. Analysis of the pump-dump-probe data suggested that the main energy donor in the slow S 1 /ICT-Chl a route is the S 1 part of the S 1 /ICT potential surface. Copyright © 2018 Elsevier B.V. All rights reserved.

Ultrafast energy transport in a first-generation coumarin-tetraphenylporphyrin dendrimer

NARCIS (Netherlands)

Hania, Pieter; Heijs, D.J.; Bowden, T.; Pugzlys, A; van Esch, J; Knoester, J; Duppen, K

2004-01-01

Energy transfer in a newly synthesized coumarin-tetraphenylporphyrin donor-acceptor system was studied by time- and frequency-resolved fluorescence spectroscopy. The energy transfer kinetics was shown to be fast (transfer time ca. 500 fs) and efficient (quantum yield ca. 97%). The influence of

Ultrafast electron transfer in all-carbon-based SWCNT-C60 donor-acceptor nanoensembles connected by poly(phenylene-ethynylene) spacers

Science.gov (United States)

Barrejón, Myriam; Gobeze, Habtom B.; Gómez-Escalonilla, María J.; Fierro, José Luis G.; Zhang, Minfang; Yudasaka, Masako; Iijima, Sumio; D'Souza, Francis; Langa, Fernando

2016-08-01

Building all-carbon based functional materials for light energy harvesting applications could be a solution to tackle and reduce environmental carbon output. However, development of such all-carbon based donor-acceptor hybrids and demonstration of photoinduced charge separation in such nanohybrids is a challenge since in these hybrids part of the carbon material should act as an electron donating or accepting photosensitizer while the second part should fulfil the role of an electron acceptor or donor. In the present work, we have successfully addressed this issue by synthesizing covalently linked all-carbon-based donor-acceptor nanoensembles using single-walled carbon nanotubes (SWCNTs) as the donor and C60 as the acceptor. The donor-acceptor entities in the nanoensembles were connected by phenylene-ethynylene spacer units to achieve better electronic communication and to vary the distance between the components. These novel SWCNT-C60 nanoensembles have been characterized by a number of techniques, including TGA, FT-IR, Raman, AFM, absorbance and electrochemical methods. The moderate number of fullerene addends present on the side-walls of the nanotubes largely preserved the electronic structure of the nanotubes. The thermodynamic feasibility of charge separation in these nanoensembles was established using spectral and electrochemical data. Finally, occurrence of ultrafast electron transfer from the excited nanotubes in these donor-acceptor nanohybrids has been established by femtosecond transient absorption studies, signifying their utility in building light energy harvesting devices.Building all-carbon based functional materials for light energy harvesting applications could be a solution to tackle and reduce environmental carbon output. However, development of such all-carbon based donor-acceptor hybrids and demonstration of photoinduced charge separation in such nanohybrids is a challenge since in these hybrids part of the carbon material should act as an

Ultrafast dynamics of colloidal semiconductor nanocrystals relevant to solar fuels production

Science.gov (United States)

Cogan, Nicole M. B.; Liu, Cunming; Qiu, Fen; Burke, Rebeckah; Krauss, Todd D.

2017-05-01

Artificial conversion of sunlight to chemical fuels has attracted attention for several decades as a potential source of clean, renewable energy. We recently found that CdSe quantum dots (QDs) and simple aqueous Ni2+ salts in the presence of a sacrificial electron donor form a highly efficient, active, and robust system for photochemical reduction of protons to molecular hydrogen. Ultrafast transient absorption spectroscopy studies of electron transfer (ET) processes from the QDs to the Ni catalysts reveal extremely fast ET, and provide a fundamental explanation for the exceptional photocatalytic H2 activity. Additionally, by studying H2 production of the Ni catalyst with CdSe/CdS nanoparticles of various structures, it was determined that surface charge density plays an important role in charge transfer and ultimately H2 production activity.

Quantum design of photosynthesis for bio-inspired solar-energy conversion

NARCIS (Netherlands)

Romero, Elisabet; Novoderezhkin, Vladimir I.; van Grondelle, Rienk

2017-01-01

Photosynthesis is the natural process that converts solar photons into energy-rich products that are needed to drive the biochemistry of life. Two ultrafast processes form the basis of photosynthesis: excitation energy transfer and charge separation. Under optimal conditions, every photon that is

Probing ultrafast changes of spin and charge density profiles with resonant XUV magnetic reflectivity at the free-electron laser FERMI

Directory of Open Access Journals (Sweden)

C. Gutt

2017-09-01

Full Text Available We report the results of resonant magnetic XUV reflectivity experiments performed at the XUV free-electron laser FERMI. Circularly polarized XUV light with the photon energy tuned to the Fe M2,3 edge is used to measure resonant magnetic reflectivities and the corresponding Q-resolved asymmetry of a Permalloy/Ta/Permalloy trilayer film. The asymmetry exhibits ultrafast changes on 240 fs time scales upon pumping with ultrashort IR laser pulses. Depending on the value of the wavevector transfer Qz, we observe both decreasing and increasing values of the asymmetry parameter, which is attributed to ultrafast changes in the vertical spin and charge density profiles of the trilayer film.

Ultrafast Thermal Transport at Interfaces

Energy Technology Data Exchange (ETDEWEB)

Cahill, David [Univ. of Illinois, Champaign, IL (United States); Murphy, Catherine [Univ. of Illinois, Champaign, IL (United States); Martin, Lane [Univ. of Illinois, Champaign, IL (United States)

2014-10-21

Our research program on Ultrafast Thermal Transport at Interfaces advanced understanding of the mesoscale science of heat conduction. At the length and time scales of atoms and atomic motions, energy is transported by interactions between single-particle and collective excitations. At macroscopic scales, entropy, temperature, and heat are the governing concepts. Key gaps in fundamental knowledge appear at the transitions between these two regimes. The transport of thermal energy at interfaces plays a pivotal role in these scientific issues. Measurements of heat transport with ultrafast time resolution are needed because picoseconds are the fundamental scales where the lack of equilibrium between various thermal excitations becomes a important factor in the transport physics. A critical aspect of our work has been the development of experimental methods and model systems that enabled more precise and sensitive investigations of nanoscale thermal transport.

Extension of Light-Harvesting Ability of Photosynthetic Light-Harvesting Complex 2 (LH2) through Ultrafast Energy Transfer from Covalently Attached Artificial Chromophores.

Science.gov (United States)

Yoneda, Yusuke; Noji, Tomoyasu; Katayama, Tetsuro; Mizutani, Naoto; Komori, Daisuke; Nango, Mamoru; Miyasaka, Hiroshi; Itoh, Shigeru; Nagasawa, Yutaka; Dewa, Takehisa

2015-10-14

Introducing appropriate artificial components into natural biological systems could enrich the original functionality. To expand the available wavelength range of photosynthetic bacterial light-harvesting complex 2 (LH2 from Rhodopseudomonas acidophila 10050), artificial fluorescent dye (Alexa Fluor 647: A647) was covalently attached to N- and C-terminal Lys residues in LH2 α-polypeptides with a molar ratio of A647/LH2 ≃ 9/1. Fluorescence and transient absorption spectroscopies revealed that intracomplex energy transfer from A647 to intrinsic chromophores of LH2 (B850) occurs in a multiexponential manner, with time constants varying from 440 fs to 23 ps through direct and B800-mediated indirect pathways. Kinetic analyses suggested that B800 chromophores mediate faster energy transfer, and the mechanism was interpretable in terms of Förster theory. This study demonstrates that a simple attachment of external chromophores with a flexible linkage can enhance the light harvesting activity of LH2 without affecting inherent functions of energy transfer, and can achieve energy transfer in the subpicosecond range. Addition of external chromophores, thus, represents a useful methodology for construction of advanced hybrid light-harvesting systems that afford solar energy in the broad spectrum.

Energy transfer properties and mechanisms

International Nuclear Information System (INIS)

1991-01-01

This report discusses the energy transfer mechanisms in azulene, benzene, toluene, and isotopomers. Also discussed is the coupled energy reservoirs model, quantum effects in energy transfer, NO 2 energy transfer, densities of states, the reactant states model, and O 3 excited electronic states

PREFACE: Ultrafast biophotonics Ultrafast biophotonics

Science.gov (United States)

Gu, Min; Reid, Derryck; Ben-Yakar, Adela

2010-08-01

The use of light to explore biology can be traced to the first observations of tissue made with early microscopes in the mid-seventeenth century, and has today evolved into the discipline which we now know as biophotonics. This field encompasses a diverse range of activities, each of which shares the common theme of exploiting the interaction of light with biological material. With the rapid advancement of ultrafast optical technologies over the last few decades, ultrafast lasers have increasingly found applications in biophotonics, to the extent that the distinctive new field of ultrafast biophotonics has now emerged, where robust turnkey ultrafast laser systems are facilitating cutting-edge studies in the life sciences to take place in everyday laboratories. The broad spectral bandwidths, precision timing resolution, low coherence and high peak powers of ultrafast optical pulses provide unique opportunities for imaging and manipulating biological systems. Time-resolved studies of bio-molecular dynamics exploit the short pulse durations from such lasers, while other applications such as optical coherence tomography benefit from the broad optical bandwidths possible by using super-continuum generation and additionally allowing for high speed imaging with speeds as high as 47 000 scans per second. Continuing progress in laser-system technology is accelerating the adoption of ultrafast techniques across the life sciences, both in research laboratories and in clinical applications, such as laser-assisted in situ keratomileusis (LASIK) eye surgery. Revolutionizing the field of optical microscopy, two-photon excitation fluorescence (TPEF) microscopy has enabled higher spatial resolution with improved depth penetration into biological specimens. Advantages of this nonlinear optical process include: reduced photo-interactions, allowing for extensive imaging time periods; simultaneously exciting multiple fluorescent molecules with only one excitation wavelength; and

Ultrafast endothermic transfer of non-radiative exciplex state to radiative excitons in polyfluorene random copolymer for blue electroluminescence

Science.gov (United States)

Moghe, Dhanashree A.; Dey, Amrita; Johnson, Kerr; Lu, L.-P.; Friend, Richard H.; Kabra, Dinesh

2018-04-01

We report a blue-emitting random copolymer (termed modified Aryl-F8) consisting of three repeat units of polydioctylfluorene (F8), Aryl-polydioctylfluorene (Aryl-F8), and an aromatic amine comonomer unit, poly(bis-N,Ν'-(4-butylphenyl)-bis-N,N'-phenyl-1,4 phenylenediamine) chemically linked to get an improved charge carrier balance without compromising on the photoluminescence (PL) quantum yield with respect to the Aryl-F8 homo-polymer. The measured photoluminescence quantum efficiency (˜70%) of the blue-emitting polymer is comparable to or greater than the individual monomer units. The time resolved PL spectra from the modified Aryl-F8 are similar to those of Arylated-poly(9,9'-dioctylfluorene-co-bis-N,N'-(4-butylphenyl)-bis-N,N'-phenyl-1,4 phenylenediamine) (PFB) even at a time scale of 100-250 ps, indicating an ultrafast energy transfer from the (Aryl-F8 or F8):Arylated-PFB interface to Arylated-PFB, i.e., endothermic transfer of non-radiative exciplex to a radiative molecular exciton. Furthermore, the presence of non-radiative exciplex is confirmed by the photoluminescence decay profile and temperature dependent PL spectra. The luminance efficiency achieved for the modified Aryl-F8 polymer light-emitting diodes is ˜11 cd A-1 with an external quantum efficiency (EQE) of ˜4.5%, whereas it is 0.05 cd/A with an EQE of ˜0.025% for Aryl-F8. Almost two orders of higher efficiency is achieved due to the improved charge carrier balance from the random copolymer without compromising on the photoluminescence yield.

High Harmonic Generation XUV Spectroscopy for Studying Ultrafast Photophysics of Coordination Complexes

Science.gov (United States)

Ryland, Elizabeth S.; Lin, Ming-Fu; Benke, Kristin; Verkamp, Max A.; Zhang, Kaili; Vura-Weis, Josh

2017-06-01

Extreme ultraviolet (XUV) spectroscopy is an inner shell technique that probes the M_{2,3}-edge excitation of atoms. Absorption of the XUV photon causes a 3p→3d transition, the energy and shape of which is directly related to the element and ligand environment. This technique is thus element-, oxidation state-, spin state-, and ligand field specific. A process called high-harmonic generation (HHG) enables the production of ultrashort (˜20fs) pulses of collimated XUV photons in a tabletop instrument. This allows transient XUV spectroscopy to be conducted as an in-lab experiment, where it was previously only possible at accelerator-based light sources. Additionally, ultrashort pulses provide the capability for unprecedented time resolution (˜50fs IRF). This technique has the capacity to serve a pivotal role in the study of electron and energy transfer processes in materials and chemical biology. I will present the XUV transient absorption instrument we have built, along with ultrafast transient M_{2,3}-edge absorption data of a series of small inorganic molecules in order to demonstrate the high specificity and time resolution of this tabletop technique as well as how our group is applying it to the study of ultrafast electronic dynamics of coordination complexes.

Short-Range Electron Transfer in Reduced Flavodoxin: Ultrafast Nonequilibrium Dynamics Coupled with Protein Fluctuations.

Science.gov (United States)

Kundu, Mainak; He, Ting-Fang; Lu, Yangyi; Wang, Lijuan; Zhong, Dongping

2018-05-03

Short-range electron transfer (ET) in proteins is an ultrafast process on the similar timescales as local protein-solvent fluctuations thus the two dynamics are coupled. Here, we use semiquinone flavodoxin and systematically characterized the photoinduced redox cycle with eleven mutations of different aromatic electron donors (tryptophan and tyrosine) and local residues to change redox properties. We observed the forward and backward ET dynamics in a few picoseconds, strongly following a stretched behavior resulting from a coupling between local environment relaxations and these ET processes. We further observed the hot vibrational-state formation through charge recombination and the subsequent cooling dynamics also in a few picoseconds. Combined with the ET studies in oxidized flavodoxin, these results coherently reveal the evolution of the ET dynamics from single to stretched exponential behaviors and thus elucidate critical timescales for the coupling. The observed hot vibration-state formation is robust and should be considered in all photoinduced back ET processes in flavoproteins.

Energy transfer in plasmonic systems

International Nuclear Information System (INIS)

Pustovit, Vitaliy N; Urbas, Augustine M; Shahbazyan, Tigran V

2014-01-01

We present our results on energy transfer between donor and acceptor molecules or quantum dots near a plasmonic nanoparticle. In such systems, the Förster resonance energy transfer is strongly modified due to plasmon-mediated coupling between donors and acceptors. The transfer efficiency is determined by a competition between transfer, radiation and dissipation that depends sensitively on system parameters. When donor and accepror spectral bands overlap with dipole surface plasmon resonance, the dominant transfer mechanism is through plasmon-enhanced radiative coupling. When transfer takes place from an ensemble of donors to an acceptor, a cooperative amplification of energy transfer takes place in a wide range of system parameters. (paper)

Ultrafast electron diffraction from non-equilibrium phonons in femtosecond laser heated Au films

Energy Technology Data Exchange (ETDEWEB)

Chase, T. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Department of Applied Physics, Stanford University, Stanford, California 94305 (United States); Trigo, M.; Reid, A. H.; Dürr, H. A. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Li, R.; Vecchione, T.; Shen, X.; Weathersby, S.; Coffee, R.; Hartmann, N.; Wang, X. J. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Reis, D. A. [Stanford Institute for Materials and Energy Sciences, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Department of Applied Physics, Stanford University, Stanford, California 94305 (United States); PULSE Institute, SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States)

2016-01-25

We use ultrafast electron diffraction to detect the temporal evolution of non-equilibrium phonons in femtosecond laser-excited ultrathin single-crystalline gold films. From the time-dependence of the Debye-Waller factor, we extract a 4.7 ps time-constant for the increase in mean-square atomic displacements. The observed increase in the diffuse scattering intensity demonstrates that the energy transfer from laser-heated electrons to phonon modes near the X and K points in the Au fcc Brillouin zone proceeds with timescales of 2.3 and 2.9 ps, respectively, faster than the Debye-Waller average mean-square displacement.

Directing the path of light-induced electron transfer at a molecular fork using vibrational excitation

Science.gov (United States)

Delor, Milan; Archer, Stuart A.; Keane, Theo; Meijer, Anthony J. H. M.; Sazanovich, Igor V.; Greetham, Gregory M.; Towrie, Michael; Weinstein, Julia A.

2017-11-01

Ultrafast electron transfer in condensed-phase molecular systems is often strongly coupled to intramolecular vibrations that can promote, suppress and direct electronic processes. Recent experiments exploring this phenomenon proved that light-induced electron transfer can be strongly modulated by vibrational excitation, suggesting a new avenue for active control over molecular function. Here, we achieve the first example of such explicit vibrational control through judicious design of a Pt(II)-acetylide charge-transfer donor-bridge-acceptor-bridge-donor 'fork' system: asymmetric 13C isotopic labelling of one of the two -C≡C- bridges makes the two parallel and otherwise identical donor→acceptor electron-transfer pathways structurally distinct, enabling independent vibrational perturbation of either. Applying an ultrafast UVpump(excitation)-IRpump(perturbation)-IRprobe(monitoring) pulse sequence, we show that the pathway that is vibrationally perturbed during UV-induced electron transfer is dramatically slowed down compared to its unperturbed counterpart. One can thus choose the dominant electron transfer pathway. The findings deliver a new opportunity for precise perturbative control of electronic energy propagation in molecular devices.

Plasmon assisted control of photo-induced excitation energy transfer in a molecular chain

Science.gov (United States)

Wang, Luxia; May, Volkhard

2017-08-01

The strong and ultrafast laser pulse excitation of a molecular chain in close vicinity to a spherical metal nano-particle (MNP) is studied theoretically. Due to local-field enhancement around the MNP, pronounced excited-state formation has to be expected for the part of the chain which is in proximity to the MNP. Here, the description of this phenomenon will be based on a uniform quantum theory of the MNP-molecule system. It accounts for local-field effects due to direct consideration of the strong excitation energy transfer coupling between the MNP and the various molecules. The molecule-MNP distances are chosen in such a way as to achieve a correct description of the MNP via dipole-plasmon excitations. Short plasmon life-times are incorporated in the framework of a density matrix approach. By extending earlier work the present description allows for multi-exciton formation and multiple dipole-plasmon excitation. The region of less intense and not-too-short optical excitation is identified as being best suited for excitation energy localization in the chain.

Cutting-Edge High-Power Ultrafast Thin Disk Oscillators

Directory of Open Access Journals (Sweden)

Thomas Südmeyer

2013-04-01

Full Text Available A growing number of applications in science and industry are currently pushing the development of ultrafast laser technologies that enable high average powers. SESAM modelocked thin disk lasers (TDLs currently achieve higher pulse energies and average powers than any other ultrafast oscillator technology, making them excellent candidates in this goal. Recently, 275 W of average power with a pulse duration of 583 fs were demonstrated, which represents the highest average power so far demonstrated from an ultrafast oscillator. In terms of pulse energy, TDLs reach more than 40 μJ pulses directly from the oscillator. In addition, another major milestone was recently achieved, with the demonstration of a TDL with nearly bandwidth-limited 96-fs long pulses. The progress achieved in terms of pulse duration of such sources enabled the first measurement of the carrier-envelope offset frequency of a modelocked TDL, which is the first key step towards full stabilization of such a source. We will present the key elements that enabled these latest results, as well as an outlook towards the next scaling steps in average power, pulse energy and pulse duration of such sources. These cutting-edge sources will enable exciting new applications, and open the door to further extending the current performance milestones.

Understanding the features in the ultrafast transient absorption spectra of CdSe quantum dots

Energy Technology Data Exchange (ETDEWEB)

Zhang, Cheng; Do, Thanh Nhut [Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371 (Singapore); Ong, Xuanwei [Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore); Chan, Yinthai [Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore 117543 (Singapore); Institute of Materials Research & Engineering, A*STAR, 2 Fusionopolis Way, Innovis, Singapore 138634 (Singapore); Tan, Howe-Siang, E-mail: howesiang@ntu.edu.sg [Division of Chemistry and Biological Chemistry, School of Physical and Mathematical Sciences, Nanyang Technological University, 21 Nanyang Link, Singapore 637371 (Singapore)

2016-12-20

We describe a model to explain the features of the ultrafast transient absorption (TA) spectra of CdSe core type quantum dots (QDs). The measured TA spectrum consists of contributions by the ground state bleach (GSB), stimulated emission (SE) and excited state absorption (ESA) processes associated with the three lowest energy transition of the QDs. We model the shapes of the GSB, SE and ESA spectral components after fits to the linear absorption. The spectral positions of the ESA components take into account the biexcitonic binding energy. In order to obtain the correct weightage of the GSB, SE and ESA components to the TA spectrum, we enumerate the set of coherence transfer pathways associated with these processes. From our fits of the experimental TA spectra of 65 Å diameter QDs, biexcitonic binding energies for the three lowest energy transitions are obtained.

Nonlinear performance of asymmetric coupler based on dual-core photonic crystal fiber: Towards sub-nanojoule solitonic ultrafast all-optical switching

Science.gov (United States)

Curilla, L.; Astrauskas, I.; Pugzlys, A.; Stajanca, P.; Pysz, D.; Uherek, F.; Baltuska, A.; Bugar, I.

2018-05-01

We demonstrate ultrafast soliton-based nonlinear balancing of dual-core asymmetry in highly nonlinear photonic crystal fiber at sub-nanojoule pulse energy level. The effect of fiber asymmetry was studied experimentally by selective excitation and monitoring of individual fiber cores at different wavelengths between 1500 nm and 1800 nm. Higher energy transfer rate to non-excited core was observed in the case of fast core excitation due to nonlinear asymmetry balancing of temporal solitons, which was confirmed by the dedicated numerical simulations based on the coupled generalized nonlinear Schrödinger equations. Moreover, the simulation results correspond qualitatively with the experimentally acquired dependences of the output dual-core extinction ratio on excitation energy and wavelength. In the case of 1800 nm fast core excitation, narrow band spectral intensity switching between the output channels was registered with contrast of 23 dB. The switching was achieved by the change of the excitation pulse energy in sub-nanojoule region. The performed detailed analysis of the nonlinear balancing of dual-core asymmetry in solitonic propagation regime opens new perspectives for the development of ultrafast nonlinear all-optical switching devices.

Energy transfers and magnetic energy growth in small-scale dynamo

KAUST Repository

Kumar, Rohit Raj

2013-12-01

In this letter we investigate the dynamics of magnetic energy growth in small-scale dynamo by studying energy transfers, mainly energy fluxes and shell-to-shell energy transfers. We perform dynamo simulations for the magnetic Prandtl number Pm = 20 on 10243 grid using the pseudospectral method. We demonstrate that the magnetic energy growth is caused by nonlocal energy transfers from the large-scale or forcing-scale velocity field to small-scale magnetic field. The peak of these energy transfers moves towards lower wave numbers as dynamo evolves, which is the reason why the integral scale of the magnetic field increases with time. The energy transfers U2U (velocity to velocity) and B2B (magnetic to magnetic) are forward and local. Copyright © EPLA, 2013.

Energy-transfer properties and mechanisms:

International Nuclear Information System (INIS)

Barker, J.R.

1988-02-01

This project continues the research on vibrational energy transfer involving large molecules. The motivation of the research is to advance knowledge concerning molecular energy in the electronic ground state so that meaningful predictions can be made. The experimental program will use several techniques on several different molecules with the aim of eliminating experimental artifacts and gaining more insight into energy transfer processes. The theoretical effort will be directed toward assessing the validity of the Biased Random Walk theory and toward developing simpler models that adequately describe the energy transfer process. 6 figs

An ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle

International Nuclear Information System (INIS)

Gu Zhiguo; Yang Shuping; Li Zaijun; Sun Xiulan; Wang Guangli; Fang Yinjun; Liu Junkang

2011-01-01

Graphical abstract: We first reported an ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since promising their electrocatalytic synergy towards glucose was achieved, the biosensor showed high sensitivity (5762.8 nA nM -1 cm -2 ), low detection limit (S/N = 3) (3 x 10 -12 M) and fast response time (0.045 s). - Abstract: The paper reported an ultrasensitive electrochemical biosensor for glucose which was based on CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since efficient electron transfer between glucose oxidase and the electrode was achieved, the biosensor showed high sensitivity (5762.8 nA nM -1 cm -2 ), low detection limit (S/N = 3) (3 x 10 -12 M), fast response time (0.045 s), wide calibration range (from 1 x 10 -11 M to 1 x 10 -8 M) and good long-term stability (26 weeks). The apparent Michaelis-Menten constant of the glucose oxidase on the medium, 5.24 x 10 -6 mM, indicates excellent bioelectrocatalytic activity of the immobilized enzyme towards glucose oxidation. Moreover, the effects of omitting graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle were also investigated. The result showed sensitivity of the biosensor is 7.67-fold better if graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle are used. This could be ascribed to improvement of the conductivity between graphene nanosheets due to introduction of gold nanoparticles, ultrafast charge transfer from CdTe-CdS core-shell quantum dot to graphene nanosheets and gold nanoparticle due to unique electrochemical properties of the CdTe-CdS core-shell quantum dot and good biocompatibility of gold nanoparticle for glucose oxidase. The biosensor is of best sensitivity in all glucose biosensors based on graphene nanomaterials up to

An ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle

Energy Technology Data Exchange (ETDEWEB)

Gu Zhiguo; Yang Shuping [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China); Li Zaijun, E-mail: zaijunli@263.net [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China); Sun Xiulan [School of Food Science and Technology, Jiangnan University, Wuxi 214122 (China); Wang Guangli [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China); Fang Yinjun [Zhejiang Zanyu Technology Co., Ltd., Hangzhou 310009 (China); Liu Junkang [School of Chemical and Material Engineering, Jiangnan University, Wuxi 214122 (China)

2011-10-30

Graphical abstract: We first reported an ultrasensitive electrochemical biosensor for glucose using CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since promising their electrocatalytic synergy towards glucose was achieved, the biosensor showed high sensitivity (5762.8 nA nM{sup -1} cm{sup -2}), low detection limit (S/N = 3) (3 x 10{sup -12} M) and fast response time (0.045 s). - Abstract: The paper reported an ultrasensitive electrochemical biosensor for glucose which was based on CdTe-CdS core-shell quantum dot as ultrafast electron transfer relay between graphene-gold nanocomposite and gold nanoparticle. Since efficient electron transfer between glucose oxidase and the electrode was achieved, the biosensor showed high sensitivity (5762.8 nA nM{sup -1} cm{sup -2}), low detection limit (S/N = 3) (3 x 10{sup -12} M), fast response time (0.045 s), wide calibration range (from 1 x 10{sup -11} M to 1 x 10{sup -8} M) and good long-term stability (26 weeks). The apparent Michaelis-Menten constant of the glucose oxidase on the medium, 5.24 x 10{sup -6} mM, indicates excellent bioelectrocatalytic activity of the immobilized enzyme towards glucose oxidation. Moreover, the effects of omitting graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle were also investigated. The result showed sensitivity of the biosensor is 7.67-fold better if graphene-gold nanocomposite, CdTe-CdS core-shell quantum dot and gold nanoparticle are used. This could be ascribed to improvement of the conductivity between graphene nanosheets due to introduction of gold nanoparticles, ultrafast charge transfer from CdTe-CdS core-shell quantum dot to graphene nanosheets and gold nanoparticle due to unique electrochemical properties of the CdTe-CdS core-shell quantum dot and good biocompatibility of gold nanoparticle for glucose oxidase. The biosensor is of best sensitivity in all glucose

Fourteenth International Conference on Ultrafast Phenomena

CERN Document Server

Kobayashi, Takayoshi; Kobayashi, Tetsuro; Nelson, Keith A; Silvestri, Sandro; Ultrafast Phenomena XIV

2005-01-01

Ultrafast Phenomena XIV presents the latest advances in ultrafast science, including ultrafast laser and measurement technology as well as studies of ultrafast phenomena. Pico-, femto-, and atosecond processes relevant in physics, chemistry, biology and engineering are presented. Ultrafast technology is now having a profound impact within a wide range of applications, among them imaging, material diagnostics, and transformation and high-speed optoelectronics. This book summarizes results presented at the 14th Ultrafast Phenomena Conference and reviews the state of the art in this important and rapidly advancing field.

Sixteenth International Conference on Ultrafast Phenomena

CERN Document Server

Corkum, Paul; Nelson, Keith A; Riedle, Eberhard; Schoenlein, Robert W; Ultrafast Phenomena XVI

2009-01-01

Ultrafast Phenomena XVI presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond and attosecond processes relevant to applications in physics, chemistry, biology, and engineering. Ultrafast technology has a profound impact in a wide range of applications, amongst them biomedical imaging, chemical dynamics, frequency standards, material processing, and ultrahigh speed communications. This book summarizes the results presented at the 16th International Conference on Ultrafast Phenomena and provides an up-to-date view of this important and rapidly advancing field.

Communication: Broad manifold of excitonic states in light-harvesting complex 1 promotes efficient unidirectional energy transfer in vivo

Science.gov (United States)

Sohail, Sara H.; Dahlberg, Peter D.; Allodi, Marco A.; Massey, Sara C.; Ting, Po-Chieh; Martin, Elizabeth C.; Hunter, C. Neil; Engel, Gregory S.

2017-10-01

In photosynthetic organisms, the pigment-protein complexes that comprise the light-harvesting antenna exhibit complex electronic structures and ultrafast dynamics due to the coupling among the chromophores. Here, we present absorptive two-dimensional (2D) electronic spectra from living cultures of the purple bacterium, Rhodobacter sphaeroides, acquired using gradient assisted photon echo spectroscopy. Diagonal slices through the 2D lineshape of the LH1 stimulated emission/ground state bleach feature reveal a resolvable higher energy population within the B875 manifold. The waiting time evolution of diagonal, horizontal, and vertical slices through the 2D lineshape shows a sub-100 fs intra-complex relaxation as this higher energy population red shifts. The absorption (855 nm) of this higher lying sub-population of B875 before it has red shifted optimizes spectral overlap between the LH1 B875 band and the B850 band of LH2. Access to an energetically broad distribution of excitonic states within B875 offers a mechanism for efficient energy transfer from LH2 to LH1 during photosynthesis while limiting back transfer. Two-dimensional lineshapes reveal a rapid decay in the ground-state bleach/stimulated emission of B875. This signal, identified as a decrease in the dipole strength of a strong transition in LH1 on the red side of the B875 band, is assigned to the rapid localization of an initially delocalized exciton state, a dephasing process that frustrates back transfer from LH1 to LH2.

Energy transfer properties and mechanisms

International Nuclear Information System (INIS)

Barker, J.R.

1993-01-01

Since no single experimental technique is the best method for energy transfer experiments, we have used both time-dependent infrared fluorescence (IRF) and time-dependent thermal lensing (TDTL) to study energy transfer in various systems. We are investigating pump-probe techniques employing resonance enhanced multiphoton ionization (REMPI). IRF was used to study benzene, azulene, and toluene. TDTL was used to study CS 2 and SO 2 (data not given for latter). Large molecule energy transfer mechanisms are discussed. 10 figs

Advanced ultrafast fiber laser sources enabled by fiber nonlinearities

International Nuclear Information System (INIS)

Liu, Wei

2017-05-01

Development of high power/energy ultrafast fiber lasers for scientific research and industrial applications is one of the most exciting fields in ultrafast optics. This thesis demonstrated new means to improve two essential properties - which are indispensable for novel applications such as high-harmonic generation (HHG) and multiphoton microscopy (MPM) - of an ultrafast fiber laser system: energy scaling capability and wavelength tunability. High photon-flux extreme ultraviolet sources enabled by HHG desire high power (>100 W), high repetition-rate (>1 MHz) ultrafast driving laser sources. We have constructed from scratch a high-power Yb-fiber laser system using the well-known chirped-pulse amplification (CPA) technique. Such a CPA system capable of producing ∝200-W average power consists of a monolithic Yb-fiber oscillator, an all-fiber stretcher, a pre-amplifier chain, a main amplifier constructed from rode-type large pitch fiber, and a diffraction-grating based compressor. To increase the HHG efficiency, ultrafast pulses with duration 130-W average power. The amplified pulses are compressed to 60-fs pulses with 100-W average power, constituting a suitable HHG driving source. MPM is a powerful biomedical imaging tool, featuring larger penetration depth while providing the capability of optical sectioning. Although femtosecond solid-state lasers have been widely accepted as the standard option as MPM driving sources, fiber-based sources have received growing research efforts due to their superior performance. In the second part of this thesis, we both theoretically and experimentally demonstrated a new method of producing wavelength widely tunable femtosecond pulses for driving MPM. We employed self-phase modulation to broaden a narrowband spectrum followed by bandpass filters to select the rightmost/leftmost spectral lobes. Widely tunable in 820-1225 nm, the resulting sources generated nearly transform-limited, ∝100 fs pulses. Using short fibers with large

Proposal to DOE Basic Energy Sciences Ultrafast X-ray science facility at the Advanced Light Source

CERN Document Server

Schönlein, R W; Alivisatos, A P; Belkacem, A; Berrah, N; Bozek, J; Bressler, C; Cavalleri, A; Chang, Z; Chergui, M; Falcone, R W; Glover, T E; Heimann, P A; Hepburn, J; Larsson, J; Lee, R W; McCusker, J; Padmore, H A; Pattison, P; Pratt, S T; Robin, D W; Schlüter, Ross D; Shank, C V; Wark, J; Zholents, A A; Zolotorev, M S

2001-01-01

We propose to develop a true user facility for ultrafast x-ray science at the Advanced Light Source. This facility will be unique in the world, and will fill a critical need for the growing ultrafast x-ray research community. The development of this facility builds upon the expertise from long-standing research efforts in ultrafast x-ray spectroscopy and the development of femtosecond x-ray sources and techniques at both the Lawrence Berkeley National Laboratory and at U.C. Berkeley. In particular, the technical feasibility of a femtosecond x-ray beamline at the ALS has already been demonstrated, and existing ultrafast laser technology will enable such a beamline to operate near the practical limit for femtosecond x-ray flux and brightness from a 3rd generation synchrotron.

Proposal to DOE Basic Energy Sciences: Ultrafast X-ray science facility at the Advanced Light Source

Energy Technology Data Exchange (ETDEWEB)

Schoenlein, Robert W.; Falcone, Roger W.; Abela, R.; Alivisatos, A.P.; Belkacem, A.; Berrah, N.; Bozek, J.; Bressler, C.; Cavalleri, A.; Chergui, M.; Glover, T.E.; Heimann, P.A.; Hepburn, J.; Larsson, J.; Lee, R.W.; McCusker, J.; Padmore, H.A.; Pattison, P.; Pratt, S.T.; Shank, C.V.; Wark, J.; Chang, Z.; Robin, D.W.; Schlueter, R.D.; Zholents, A.A.; Zolotorev, M.S.

2001-12-12

We propose to develop a true user facility for ultrafast x-ray science at the Advanced Light Source. This facility will be unique in the world, and will fill a critical need for the growing ultrafast x-ray research community. The development of this facility builds upon the expertise from long-standing research efforts in ultrafast x-ray spectroscopy and the development of femtosecond x-ray sources and techniques at both the Lawrence Berkeley National Laboratory and at U.C. Berkeley. In particular, the technical feasibility of a femtosecond x-ray beamline at the ALS has already been demonstrated, and existing ultrafast laser technology will enable such a beamline to operate near the practical limit for femtosecond x-ray flux and brightness from a 3rd generation synchrotron.

Proposal to DOE Basic Energy Sciences: Ultrafast X-ray science facility at the Advanced Light Source

International Nuclear Information System (INIS)

Schoenlein, Robert W.; Falcone, Roger W.; Abela, R.; Alivisatos, A.P.; Belkacem, A.; Berrah, N.; Bozek, J.; Bressler, C.; Cavalleri, A.; Chergui, M.; Glover, T.E.; Heimann, P.A.; Hepburn, J.; Larsson, J.; Lee, R.W.; McCusker, J.; Padmore, H.A.; Pattison, P.; Pratt, S.T.; Shank, C.V.; Wark, J.; Chang, Z.; Robin, D.W.; Schlueter, R.D.; Zholents, A.A.; Zolotorev, M.S.

2001-01-01

We propose to develop a true user facility for ultrafast x-ray science at the Advanced Light Source. This facility will be unique in the world, and will fill a critical need for the growing ultrafast x-ray research community. The development of this facility builds upon the expertise from long-standing research efforts in ultrafast x-ray spectroscopy and the development of femtosecond x-ray sources and techniques at both the Lawrence Berkeley National Laboratory and at U.C. Berkeley. In particular, the technical feasibility of a femtosecond x-ray beamline at the ALS has already been demonstrated, and existing ultrafast laser technology will enable such a beamline to operate near the practical limit for femtosecond x-ray flux and brightness from a 3rd generation synchrotron

Nanoparticle size and morphology control using ultrafast laser induced forward transfer of Ni thin films

Energy Technology Data Exchange (ETDEWEB)

Murphy, Ryan D. [Applied Physics Program, University of Michigan, Ann Arbor, Michigan 48109 (United States); Abere, Michael J.; Schrider, Keegan J.; Yalisove, Steven M. [Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109 (United States); Torralva, Ben [Department of Atmospheric, Oceanic and Space Sciences, University of Michigan, Ann Arbor, Michigan 48109 (United States)

2013-08-26

We have developed a nanoparticle (NP) printing technique using Ni thin film lift-off from glass substrates after ultrafast irradiation in air. Unique interactions of ultrafast laser pulses with thin films allow for control over NP faceting and size distributions. Control is achieved by changing the laser fluence, film thickness, and film-substrate distance. We demonstrate 20 nm Ni film removal from substrates and rapid NP printing, with size distributions centered at a 6 nm diameter. When the Ni film thickness is lowered to 10 nm, NPs are printed with distributions peaked at a 2 nm diameter.

Far-field RF energy transfer and harvesting

NARCIS (Netherlands)

Visser, H.J.; Vullers, R.; Briand, D.; Yeatman, E.; Roundy, S.

2015-01-01

This chapter deals with radio frequency (RF) energy transfer over a distance. After explaining the differences between nonradiative and radiative RF energy transfer, the chapter gives definitions for transfer and harvesting. Nonradiative RF energy transfer is mostly employed in inductive systems,

Resonance Energy Transfer Molecular Imaging Application in Biomedicine

Directory of Open Access Journals (Sweden)

NIE Da-hong1,2;TANG Gang-hua1,3

2016-11-01

Full Text Available Resonance energy transfer molecular imaging (RETI can markedly improve signal intensity and tissue penetrating capacity of optical imaging, and have huge potential application in the deep-tissue optical imaging in vivo. Resonance energy transfer (RET is an energy transition from the donor to an acceptor that is in close proximity, including non-radiative resonance energy transfer and radiative resonance energy transfer. RETI is an optical imaging technology that is based on RET. RETI mainly contains fluorescence resonance energy transfer imaging (FRETI, bioluminescence resonance energy transfer imaging (BRETI, chemiluminescence resonance energy transfer imaging (CRETI, and radiative resonance energy transfer imaging (RRETI. RETI is the hot field of molecular imaging research and has been widely used in the fields of biology and medicine. This review mainly focuses on RETI principle and application in biomedicine.

Real-time observation of ultrafast electron injection at graphene–Zn porphyrin interfaces

KAUST Repository

Masih, Dilshad

2015-02-25

We report on the ultrafast interfacial electron transfer ( ET) between zinc( II) porphyrin ( ZnTMPyP) and negatively charged graphene carboxylate ( GC) using state- of- the- art femtosecond laser spectroscopy with broadband capabilities. The steady- state interaction between GC and ZnTMPyP results in a red- shifted absorption spectrum, providing a clear indication for the binding affinity between ZnTMPyP and GC via electrostatic and p- p stacking interactions. Ultrafast transient absorption ( TA) spectra in the absence and presence of three different GC concentrations reveal ( i) the ultrafast formation of singlet excited ZnTMPyP*, which partially relaxes into a long- lived triplet state, and ( ii) ET from the singlet excited ZnTMPyP* to GC, forming ZnTMPyP + and GC , as indicated by a spectral feature at 650- 750 nm, which is attributed to a ZnTMPyP radical cation resulting from the ET process.

Controlled ultrafast transfer and stability degree of generalized coherent states of a kicked two-level ion

Science.gov (United States)

Chen, Hao; Kong, Chao; Hai, Wenhua

2018-06-01

We investigate quantum dynamics of a two-level ion trapped in the Lamb-Dicke regime of a δ -kicked optical lattice, based on the exact generalized coherent states rotated by a π / 2 pulse of Ramsey type experiment. The spatiotemporal evolutions of the spin-motion entangled states in different parameter regions are illustrated, and the parameter regions of different degrees of quantum stability described by the quantum fidelity are found. Time evolutions of the probability for the ion being in different pseudospin states reveal that the ultrafast entanglement generation and population transfers of the system can be analytically controlled by managing the laser pulses. The probability in an initially disentangled state shows periodic collapses (entanglement) and revivals (de-entanglement). Reduction of the stability degree results in enlarging the period of de-entanglement, while the instability and potential chaos will cause the sustained entanglement. The results could be justified experimentally in the existing setups and may be useful in engineering quantum dynamics for quantum information processing.

Ultrafast Ultrasound Imaging With Cascaded Dual-Polarity Waves.

Science.gov (United States)

Zhang, Yang; Guo, Yuexin; Lee, Wei-Ning

2018-04-01

Ultrafast ultrasound imaging using plane or diverging waves, instead of focused beams, has advanced greatly the development of novel ultrasound imaging methods for evaluating tissue functions beyond anatomical information. However, the sonographic signal-to-noise ratio (SNR) of ultrafast imaging remains limited due to the lack of transmission focusing, and thus insufficient acoustic energy delivery. We hereby propose a new ultrafast ultrasound imaging methodology with cascaded dual-polarity waves (CDWs), which consists of a pulse train with positive and negative polarities. A new coding scheme and a corresponding linear decoding process were thereby designed to obtain the recovered signals with increased amplitude, thus increasing the SNR without sacrificing the frame rate. The newly designed CDW ultrafast ultrasound imaging technique achieved higher quality B-mode images than coherent plane-wave compounding (CPWC) and multiplane wave (MW) imaging in a calibration phantom, ex vivo pork belly, and in vivo human back muscle. CDW imaging shows a significant improvement in the SNR (10.71 dB versus CPWC and 7.62 dB versus MW), penetration depth (36.94% versus CPWC and 35.14% versus MW), and contrast ratio in deep regions (5.97 dB versus CPWC and 5.05 dB versus MW) without compromising other image quality metrics, such as spatial resolution and frame rate. The enhanced image qualities and ultrafast frame rates offered by CDW imaging beget great potential for various novel imaging applications.

Unlocking the Constraints of Cyanobacterial Productivity: Acclimations Enabling Ultrafast Growth

Energy Technology Data Exchange (ETDEWEB)

Bernstein, Hans C.; McClure, Ryan S.; Hill, Eric A.; Markillie, Lye Meng; Chrisler, William B.; Romine, Margie F.; McDermott, Jason E.; Posewitz, Matthew C.; Bryant, Donald A.; Konopka, Allan E.; Fredrickson, James K.; Beliaev, Alexander S.

2016-07-26

Harnessing the metabolic potential of photosynthetic microbes for next-generation biotechnology objectives requires detailed scientific understanding of the physiological constraints and regulatory controls affecting carbon partitioning between biomass, metabolite storage pools, and bioproduct synthesis. We dissected the cellular mechanisms underlying the remarkable physiological robustness of the euryhaline unicellular cyanobacteriumSynechococcussp. strain PCC 7002 (Synechococcus7002) and identify key mechanisms that allow cyanobacteria to achieve unprecedented photoautotrophic productivities (~2.5-h doubling time). Ultrafast growth ofSynechococcus7002 was supported by high rates of photosynthetic electron transfer and linked to significantly elevated transcription of precursor biosynthesis and protein translation machinery. Notably, no growth or photosynthesis inhibition signatures were observed under any of the tested experimental conditions. Finally, the ultrafast growth inSynechococcus7002 was also linked to a 300% expansion of average cell volume. We hypothesize that this cellular adaptation is required at high irradiances to support higher cell division rates and reduce deleterious effects, corresponding to high light, through increased carbon and reductant sequestration.

IMPORTANCEEfficient coupling between photosynthesis and productivity is central to the development of biotechnology based on solar energy. Therefore, understanding the factors constraining maximum rates of carbon processing is necessary to identify regulatory mechanisms and devise strategies to overcome productivity constraints. Here, we interrogate the molecular mechanisms that operate at a systems level to allow cyanobacteria to achieve ultrafast growth. This was done by considering growth and photosynthetic kinetics with global transcription patterns. We have delineated

Energy transfers and magnetic energy growth in small-scale dynamo

KAUST Repository

Kumar, Rohit Raj; Verma, Mahendra K.; Samtaney, Ravi

2013-01-01

In this letter we investigate the dynamics of magnetic energy growth in small-scale dynamo by studying energy transfers, mainly energy fluxes and shell-to-shell energy transfers. We perform dynamo simulations for the magnetic Prandtl number Pm = 20

Ultrafast photoinduced charge separation in metal-semiconductor nanohybrids.

Science.gov (United States)

Mongin, Denis; Shaviv, Ehud; Maioli, Paolo; Crut, Aurélien; Banin, Uri; Del Fatti, Natalia; Vallée, Fabrice

2012-08-28

Hybrid nano-objects formed by two or more disparate materials are among the most promising and versatile nanosystems. A key parameter in their properties is interaction between their components. In this context we have investigated ultrafast charge separation in semiconductor-metal nanohybrids using a model system of gold-tipped CdS nanorods in a matchstick architecture. Experiments are performed using an optical time-resolved pump-probe technique, exciting either the semiconductor or the metal component of the particles, and probing the light-induced change of their optical response. Electron-hole pairs photoexcited in the semiconductor part of the nanohybrids are shown to undergo rapid charge separation with the electron transferred to the metal part on a sub-20 fs time scale. This ultrafast gold charging leads to a transient red-shift and broadening of the metal surface plasmon resonance, in agreement with results for free clusters but in contrast to observation for static charging of gold nanoparticles in liquid environments. Quantitative comparison with a theoretical model is in excellent agreement with the experimental results, confirming photoexcitation of one electron-hole pair per nanohybrid followed by ultrafast charge separation. The results also point to the utilization of such metal-semiconductor nanohybrids in light-harvesting applications and in photocatalysis.

The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales (A 'Life at the Frontiers of Energy Research' contest entry from the 2011 Energy Frontier Research Centers (EFRCs) Summit and Forum)

International Nuclear Information System (INIS)

Mao, Ho-kwang

2011-01-01

'The Behavior of Hydrogen Under Extreme Conditions on Ultrafast Timescales ' was submitted by the Center for Energy Frontier Research in Extreme Environments (EFree) to the 'Life at the Frontiers of Energy Research' video contest at the 2011 Science for Our Nation's Energy Future: Energy Frontier Research Centers (EFRCs) Summit and Forum. Twenty-six EFRCs created short videos to highlight their mission and their work. EFree is directed by Ho-kwang Mao at the Carnegie Institute of Washington and is a partnership of scientists from thirteen institutions.The Office of Basic Energy Sciences in the U.S. Department of Energy's Office of Science established the 46 Energy Frontier Research Centers (EFRCs) in 2009. These collaboratively-organized centers conduct fundamental research focused on 'grand challenges' and use-inspired 'basic research needs' recently identified in major strategic planning efforts by the scientific community. The overall purpose is to accelerate scientific progress toward meeting the nation's critical energy challenges. The mission of Energy Frontier Research in Extreme Environments is 'to accelerate the discovery and creation of energy-relevant materials using extreme pressures and temperatures.' Research topics are: catalysis (CO 2 , water), photocatalysis, solid state lighting, optics, thermelectric, phonons, thermal conductivity, solar electrodes, fuel cells, superconductivity, extreme environment, radiation effects, defects, spin dynamics, CO 2 (capture, convert, store), greenhouse gas, hydrogen (fuel, storage), ultrafast physics, novel materials synthesis, and defect tolerant materials.

Design and commissioning of an aberration-corrected ultrafast spin-polarized low energy electron microscope with multiple electron sources.

Science.gov (United States)

Wan, Weishi; Yu, Lei; Zhu, Lin; Yang, Xiaodong; Wei, Zheng; Liu, Jefferson Zhe; Feng, Jun; Kunze, Kai; Schaff, Oliver; Tromp, Ruud; Tang, Wen-Xin

2017-03-01

We describe the design and commissioning of a novel aberration-corrected low energy electron microscope (AC-LEEM). A third magnetic prism array (MPA) is added to the standard AC-LEEM with two prism arrays, allowing the incorporation of an ultrafast spin-polarized electron source alongside the standard cold field emission electron source, without degrading spatial resolution. The high degree of symmetries of the AC-LEEM are utilized while we design the electron optics of the ultrafast spin-polarized electron source, so as to minimize the deleterious effect of time broadening, while maintaining full control of electron spin. A spatial resolution of 2nm and temporal resolution of 10ps (ps) are expected in the future time resolved aberration-corrected spin-polarized LEEM (TR-AC-SPLEEM). The commissioning of the three-prism AC-LEEM has been successfully finished with the cold field emission source, with a spatial resolution below 2nm. Copyright © 2017 Elsevier B.V. All rights reserved.

Real-Time Observation of Ultrafast Intraband Relaxation and Exciton Multiplication in PbS Quantum Dots

KAUST Repository

El-Ballouli, Ala’a O.

2014-03-19

We examine ultrafast intraconduction band relaxation and multiple-exciton generation (MEG) in PbS quantum dots (QDs) using transient absorption spectroscopy with 120 fs temporal resolution. The intraconduction band relaxation can be directly and excellently resolved spectrally and temporally by applying broadband pump-probe spectroscopy to excite and detect the wavelengths around the exciton absorption peak, which is located in the near-infrared region. The time-resolved data unambiguously demonstrate that the intraband relaxation time progressively increases as the pump-photon energy increases. Moreover, the relaxation time becomes much shorter as the size of the QDs decreases, indicating the crucial role of spatial confinement in the intraband relaxation process. Additionally, our results reveal the systematic scaling of the intraband relaxation time with both excess energy above the effective energy band gap and QD size. We also assess MEG in different sizes of the QDs. Under the condition of high-energy photon excitation, which is well above the MEG energy threshold, ultrafast bleach recovery due to the nonradiative Auger recombination of the multiple electron-hole pairs provides conclusive experimental evidence for the presence of MEG. For instance, we achieved quantum efficiencies of 159, 129 and 106% per single-absorbed photon at pump photoexcition of three times the band gap for QDs with band gaps of 880 nm (1.41 eV), 1000 nm (1.24 eV) and 1210 nm (1.0 eV), respectively. These findings demonstrate clearly that the efficiency of transferring excess photon energy to carrier multiplication is significantly increased in smaller QDs compared with larger ones. Finally, we discuss the Auger recombination dynamics of the multiple electron-hole pairs as a function of QD size.

Advanced ultrafast fiber laser sources enabled by fiber nonlinearities

Energy Technology Data Exchange (ETDEWEB)

Liu, Wei

2017-05-15

Development of high power/energy ultrafast fiber lasers for scientific research and industrial applications is one of the most exciting fields in ultrafast optics. This thesis demonstrated new means to improve two essential properties - which are indispensable for novel applications such as high-harmonic generation (HHG) and multiphoton microscopy (MPM) - of an ultrafast fiber laser system: energy scaling capability and wavelength tunability. High photon-flux extreme ultraviolet sources enabled by HHG desire high power (>100 W), high repetition-rate (>1 MHz) ultrafast driving laser sources. We have constructed from scratch a high-power Yb-fiber laser system using the well-known chirped-pulse amplification (CPA) technique. Such a CPA system capable of producing ∝200-W average power consists of a monolithic Yb-fiber oscillator, an all-fiber stretcher, a pre-amplifier chain, a main amplifier constructed from rode-type large pitch fiber, and a diffraction-grating based compressor. To increase the HHG efficiency, ultrafast pulses with duration <60 fs are highly desired. We proposed and demonstrated a novel amplification technique, named as pre-chirp managed amplification (PCMA). We successfully constructed an Yb-fiber based PCMA system that outputs 75-MHz spectrally broadened pulses with >130-W average power. The amplified pulses are compressed to 60-fs pulses with 100-W average power, constituting a suitable HHG driving source. MPM is a powerful biomedical imaging tool, featuring larger penetration depth while providing the capability of optical sectioning. Although femtosecond solid-state lasers have been widely accepted as the standard option as MPM driving sources, fiber-based sources have received growing research efforts due to their superior performance. In the second part of this thesis, we both theoretically and experimentally demonstrated a new method of producing wavelength widely tunable femtosecond pulses for driving MPM. We employed self-phase modulation

Ultrafast control and monitoring of material properties using terahertz pulses

Energy Technology Data Exchange (ETDEWEB)

Bowlan, Pamela Renee [Los Alamos National Lab. (LANL), Los Alamos, NM (United States). Lab. for Ultrafast Materials Optical Science (LUMOS)

2016-05-02

These are a set of slides on ultrafast control and monitoring of material properties using terahertz pulses. A few of the topics covered in these slides are: How fast is a femtosecond (fs), Different frequencies probe different properties of molecules or solids, What can a THz pulse do to a material, Ultrafast spectroscopy, Generating and measuring ultrashort THz pulses, Tracking ultrafast spin dynamics in antiferromagnets through spin wave resonances, Coherent two-dimensional THz spectroscopy, and Probing vibrational dynamics at a surface. Conclusions are: Coherent two-dimensional THz spectroscopy: a powerful approach for studying coherence and dynamics of low energy resonances. Applying this to graphene we investigated the very strong THz light mater interaction which dominates over scattering. Useful for studying coupled excitations in multiferroics and monitoring chemical reactions. Also, THz-pump, SHG-probe spectoscopy: an ultrafast, surface sensitive probe of atomic-scale symmetry changes and nonlinear phonon dymanics. We are using this in Bi₂Se₃ to investigate the nonlinear surface phonon dynamics. This is potentially very useful for studying catalysis.

Transfer of energy in an atom

International Nuclear Information System (INIS)

Chemin, J.F.

2001-01-01

In most cases the nucleus does not interact with the electron cloud because its energy range is far higher, but in some rare cases electrons from the electron cloud and the nucleus may exchange energy: an electron may de-excite by transferring a part of its energy to the nucleus that becomes itself excited (nuclear excitation by electronic transfer or NEET), conversely electrons can receive energy from the nucleus (bound internal conversion or BIC). For the first time both energy transfers have been observed: a BIC process on a tellurium-125 atom by a French team and a NEET process on a gold-197 atom by a Japanese team. (A.C.)

Wireless energy transfer through non-resonant magnetic coupling

DEFF Research Database (Denmark)

Peng, Liang; Breinbjerg, Olav; Mortensen, Asger

2010-01-01

could be properly designed to minimize undesired energy dissipation in the source coil when the power receiver is out of the range. Our basic observation paves the way for more flexible design and fabrication of non-resonant mid-range wireless energy transfer systems, thus potentially impacting......We demonstrate by theoretical analysis and experimental verification that mid-range wireless energy transfer systems may take advantage of de-tuned coupling devices, without jeopardizing the energy transfer efficiency. Allowing for a modest de-tuning of the source coil, energy transfer systems...... practical implementations of wireless energy transfer....

Ultrafast Outflows: Galaxy-scale Active Galactic Nucleus Feedback

Science.gov (United States)

Wagner, A. Y.; Umemura, M.; Bicknell, G. V.

2013-01-01

We show, using global three-dimensional grid-based hydrodynamical simulations, that ultrafast outflows (UFOs) from active galactic nuclei (AGNs) result in considerable feedback of energy and momentum into the interstellar medium (ISM) of the host galaxy. The AGN wind interacts strongly with the inhomogeneous, two-phase ISM consisting of dense clouds embedded in a tenuous, hot, hydrostatic medium. The outflow floods through the intercloud channels, sweeps up the hot ISM, and ablates and disperses the dense clouds. The momentum of the UFO is primarily transferred to the dense clouds via the ram pressure in the channel flow, and the wind-blown bubble evolves in the energy-driven regime. Any dependence on UFO opening angle disappears after the first interaction with obstructing clouds. On kpc scales, therefore, feedback by UFOs operates similarly to feedback by relativistic AGN jets. Negative feedback is significantly stronger if clouds are distributed spherically rather than in a disk. In the latter case, the turbulent backflow of the wind drives mass inflow toward the central black hole. Considering the common occurrence of UFOs in AGNs, they are likely to be important in the cosmological feedback cycles of galaxy formation.

ULTRAFAST OUTFLOWS: GALAXY-SCALE ACTIVE GALACTIC NUCLEUS FEEDBACK

Energy Technology Data Exchange (ETDEWEB)

Wagner, A. Y.; Umemura, M. [Center for Computational Sciences, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki, 305-8577 (Japan); Bicknell, G. V., E-mail: ayw@ccs.tsukuba.ac.jp [Research School of Astronomy and Astrophysics, Australian National University, ACT 2611 (Australia)

2013-01-20

We show, using global three-dimensional grid-based hydrodynamical simulations, that ultrafast outflows (UFOs) from active galactic nuclei (AGNs) result in considerable feedback of energy and momentum into the interstellar medium (ISM) of the host galaxy. The AGN wind interacts strongly with the inhomogeneous, two-phase ISM consisting of dense clouds embedded in a tenuous, hot, hydrostatic medium. The outflow floods through the intercloud channels, sweeps up the hot ISM, and ablates and disperses the dense clouds. The momentum of the UFO is primarily transferred to the dense clouds via the ram pressure in the channel flow, and the wind-blown bubble evolves in the energy-driven regime. Any dependence on UFO opening angle disappears after the first interaction with obstructing clouds. On kpc scales, therefore, feedback by UFOs operates similarly to feedback by relativistic AGN jets. Negative feedback is significantly stronger if clouds are distributed spherically rather than in a disk. In the latter case, the turbulent backflow of the wind drives mass inflow toward the central black hole. Considering the common occurrence of UFOs in AGNs, they are likely to be important in the cosmological feedback cycles of galaxy formation.

ULTRAFAST OUTFLOWS: GALAXY-SCALE ACTIVE GALACTIC NUCLEUS FEEDBACK

International Nuclear Information System (INIS)

Wagner, A. Y.; Umemura, M.; Bicknell, G. V.

2013-01-01

We show, using global three-dimensional grid-based hydrodynamical simulations, that ultrafast outflows (UFOs) from active galactic nuclei (AGNs) result in considerable feedback of energy and momentum into the interstellar medium (ISM) of the host galaxy. The AGN wind interacts strongly with the inhomogeneous, two-phase ISM consisting of dense clouds embedded in a tenuous, hot, hydrostatic medium. The outflow floods through the intercloud channels, sweeps up the hot ISM, and ablates and disperses the dense clouds. The momentum of the UFO is primarily transferred to the dense clouds via the ram pressure in the channel flow, and the wind-blown bubble evolves in the energy-driven regime. Any dependence on UFO opening angle disappears after the first interaction with obstructing clouds. On kpc scales, therefore, feedback by UFOs operates similarly to feedback by relativistic AGN jets. Negative feedback is significantly stronger if clouds are distributed spherically rather than in a disk. In the latter case, the turbulent backflow of the wind drives mass inflow toward the central black hole. Considering the common occurrence of UFOs in AGNs, they are likely to be important in the cosmological feedback cycles of galaxy formation.

Ultrafast MR Imaging in Pediatric Neuroradiology

International Nuclear Information System (INIS)

Singh, R.K.; Smith, J.T.; Wilkinson, I.D.; Griffiths, P.D.

2003-01-01

Purpose: To compare the diagnostic information obtained from ultrafast MR imaging with standard MR imaging techniques in pediatric neuroradiology. The goal was to judge whether ultrafast methods can be used to replace standard methods and reduce the need for sedation or general anesthesia as a result of the considerably shorter scan times. Material and Methods: Our prospective study involved 125 patients. Routine clinical imaging was performed along with two ultrafast methods. Single shot fast spin echo (SSFSE) was used to give T2-weighted images and an echo planar imaging (EPI) sequence to provide a T1-weighted images. The ultrafast images were presented to an experienced neuro radiologist who was also given the information present on the initial referral card. These reports based on the ultrafast images were then compared with the formal radiologic report made solely on the basis of the standard imaging. Results: The overall sensitivity and specificity for ultrafast imaging when compared to the reference standard were 78% and 98% with positive and negative predictive values of 98% and 76%. Pathologies characterized by small areas of subtle T2 prolongation were difficult or impossible to see on the ultrafast images but otherwise they provided reliable information. Conclusions: This paper demonstrates that ultrafast MR imaging can diagnose many pediatric intracranial abnormalities as well as standard methods. Anatomic resolution limits its capacity to define subtle developmental anomalies and contrast resolution limitations of the ultrafast methods reduce the detection of pathology characterized by subtle T2 prolongation

Stray energy transfer during endoscopy.

Science.gov (United States)

Jones, Edward L; Madani, Amin; Overbey, Douglas M; Kiourti, Asimina; Bojja-Venkatakrishnan, Satheesh; Mikami, Dean J; Hazey, Jeffrey W; Arcomano, Todd R; Robinson, Thomas N

2017-10-01

Endoscopy is the standard tool for the evaluation and treatment of gastrointestinal disorders. While the risk of complication is low, the use of energy devices can increase complications by 100-fold. The mechanism of increased injury and presence of stray energy is unknown. The purpose of the study was to determine if stray energy transfer occurs during endoscopy and if so, to define strategies to minimize the risk of energy complications. A gastroscope was introduced into the stomach of an anesthetized pig. A monopolar generator delivered energy for 5 s to a snare without contacting tissue or the endoscope itself. The endoscope tip orientation, energy device type, power level, energy mode, and generator type were varied to mimic in vivo use. The primary outcome (stray current) was quantified as the change in tissue temperature (°C) from baseline at the tissue closest to the tip of the endoscope. Data were reported as mean ± standard deviation. Using the 60 W coag mode while changing the orientation of the endoscope tip, tissue temperature increased by 12.1 ± 3.5 °C nearest the camera lens (p energy transfer (p = 0.04 and p = 0.002, respectively) as did utilizing the low-voltage cut mode (6.6 ± 0.5 °C, p energy transfer compared to a standard generator (1.5 ± 3.5 °C vs. 9.5 ± 0.8 °C, p energy is transferred within the endoscope during the activation of common energy devices. This could result in post-polypectomy syndrome, bleeding, or perforation outside of the endoscopist's view. Decreasing the power, utilizing low-voltage modes and/or an impedance-monitoring generator can decrease the risk of complication.

Energy transfer in turbulence under rotation

Science.gov (United States)

Buzzicotti, Michele; Aluie, Hussein; Biferale, Luca; Linkmann, Moritz

2018-03-01

It is known that rapidly rotating turbulent flows are characterized by the emergence of simultaneous upscale and downscale energy transfer. Indeed, both numerics and experiments show the formation of large-scale anisotropic vortices together with the development of small-scale dissipative structures. However the organization of interactions leading to this complex dynamics remains unclear. Two different mechanisms are known to be able to transfer energy upscale in a turbulent flow. The first is characterized by two-dimensional interactions among triads lying on the two-dimensional, three-component (2D3C)/slow manifold, namely on the Fourier plane perpendicular to the rotation axis. The second mechanism is three-dimensional and consists of interactions between triads with the same sign of helicity (homochiral). Here, we present a detailed numerical study of rotating flows using a suite of high-Reynolds-number direct numerical simulations (DNS) within different parameter regimes to analyze both upscale and downscale cascade ranges. We find that the upscale cascade at wave numbers close to the forcing scale is generated by increasingly dominant homochiral interactions which couple the three-dimensional bulk and the 2D3C plane. This coupling produces an accumulation of energy in the 2D3C plane, which then transfers energy to smaller wave numbers thanks to the two-dimensional mechanism. In the forward cascade range, we find that the energy transfer is dominated by heterochiral triads and is dominated primarily by interaction within the fast manifold where kz≠0 . We further analyze the energy transfer in different regions in the real-space domain. In particular, we distinguish high-strain from high-vorticity regions and we uncover that while the mean transfer is produced inside regions of strain, the rare but extreme events of energy transfer occur primarily inside the large-scale column vortices.

Targeting Low-Energy Ballistic Lunar Transfers

Science.gov (United States)

Parker, Jeffrey S.

2010-01-01

Numerous low-energy ballistic transfers exist between the Earth and Moon that require less fuel than conventional transfers, but require three or more months of transfer time. An entirely ballistic lunar transfer departs the Earth from a particular declination at some time in order to arrive at the Moon at a given time along a desirable approach. Maneuvers may be added to the trajectory in order to adjust the Earth departure to meet mission requirements. In this paper, we characterize the (Delta)V cost required to adjust a low-energy ballistic lunar transfer such that a spacecraft may depart the Earth at a desirable declination, e.g., 28.5(white bullet), on a designated date. This study identifies the optimal locations to place one or two maneuvers along a transfer to minimize the (Delta)V cost of the transfer. One practical application of this study is to characterize the launch period for a mission that aims to launch from a particular launch site, such as Cape Canaveral, Florida, and arrive at a particular orbit at the Moon on a given date using a three-month low-energy transfer.

Ultrafast demagnetization enhancement in CoFeB/MgO/CoFeB magnetic tunneling junction driven by spin tunneling current.

Science.gov (United States)

He, Wei; Zhu, Tao; Zhang, Xiang-Qun; Yang, Hai-Tao; Cheng, Zhao-Hua

2013-10-07

The laser-induced ultrafast demagnetization of CoFeB/MgO/CoFeB magnetic tunneling junction is exploited by time-resolved magneto-optical Kerr effect (TRMOKE) for both the parallel state (P state) and the antiparallel state (AP state) of the magnetizations between two magnetic layers. It was observed that the demagnetization time is shorter and the magnitude of demagnetization is larger in the AP state than those in the P state. These behaviors are attributed to the ultrafast spin transfer between two CoFeB layers via the tunneling of hot electrons through the MgO barrier. Our observation indicates that ultrafast demagnetization can be engineered by the hot electrons tunneling current. It opens the door to manipulate the ultrafast spin current in magnetic tunneling junctions.

Ultrafast vortex core dynamics investigated by finite-element micromagnetic simulations

Energy Technology Data Exchange (ETDEWEB)

Gliga, Sebastian

2010-07-01

The investigations carried out in this thesis concern the ultrafast dynamics of a fundamental micromagnetic configuration: the vortex. Over the past decade, a detailed understanding of the dynamic and static properties of such magnetic nanostructures has been achieved as a result of close interplay between experiments, theory and numeric simulations. Here, micromagnetic simulations were performed based on the finite-element method. The vortex structure arises in laterally-confined ferromagnets, in particular in thin-film elements, and is characterized by an in-plane curling of the magnetic moments around a very stable and narrow core. In the present study, a novel process in micromagnetism was found: the ultrafast reversal of the vortex core. The possibility of easily switching the core orientation by means of short in-plane field pulses is surprising in view of the very high stability of the core. Moreover, the simulations presented here showed that this reversal process unfolds on a time scale of only a few tens of picoseconds, which leads to the prediction of the fastest and most complex micromagnetic reversal process known to date. Indeed, the vortex core is not merely switched: it is destroyed and recreated in the immediate vicinity with an opposite direction. This is mediated by a rapid sequence of vortex-antivortex pair creation and annihilation subprocesses and results in a sudden burst-like emission of spin waves. Equally fascinating is the ultrafast dynamics of an isolated magnetic antivortex, the topological counterpart of the vortex. The simulations performed here showed that the static complementarity between vortices and antivortices is equally reflected in their ultrafast dynamics, which leads to the reversal of the antivortex core. A promising means for the control of the magnetization on the nanoscale consists in exploiting the spin-transfer torque effect. The study of the current-induced dynamics of vortices showed that the core reversal can be

Ultrafast Structural Dynamics in InSb Probed by Time-Resolved X-Ray Diffraction

International Nuclear Information System (INIS)

Chin, A.H.; Shank, C.V.; Chin, A.H.; Schoenlein, R.W.; Shank, C.V.; Glover, T.E.; Leemans, W.P.; Balling, P.

1999-01-01

Ultrafast structural dynamics in laser-perturbed InSb are studied using time-resolved x-ray diffraction with a novel femtosecond x-ray source. We report the first observation of a delay in the onset of lattice expansion, which we attribute to energy relaxation processes and lattice strain propagation. In addition, we observe direct indications of ultrafast disordering on a subpicosecond time scale. copyright 1999 The American Physical Society

Low-Energy Ballistic Transfers to Lunar Halo Orbits

Science.gov (United States)

Parker, Jeffrey S.

2009-01-01

Recent lunar missions have begun to take advantage of the benefits of low-energy ballistic transfers between the Earth and the Moon rather than implementing conventional Hohmann-like lunar transfers. Both Artemis and GRAIL plan to implement low-energy lunar transfers in the next few years. This paper explores the characteristics and potential applications of many different families of low-energy ballistic lunar transfers. The transfers presented here begin from a wide variety of different orbits at the Earth and follow several different distinct pathways to the Moon. This paper characterizes these pathways to identify desirable low-energy lunar transfers for future lunar missions.

Laser induced energy transfer

International Nuclear Information System (INIS)

Falcone, R.W.

1979-01-01

Two related methods of rapidly transferring stored energy from one excited chemical species to another are described. The first of these, called a laser induced collision, involves a reaction in which the energy balance is met by photons from an intense laser beam. A collision cross section of ca 10 - 17 cm 2 was induced in an experiment which demonstrated the predicted dependence of the cross section on wavelength and power density of the applied laser. A second type of laser induced energy transfer involves the inelastic scattering of laser radiation from energetically excited atoms, and subsequent absorption of the scattered light by a second species. The technique of producing the light, ''anti-Stokes Raman'' scattering of visible and infrared wavelength laser photons, is shown to be an efficient source of narrow bandwidth, high brightness, tunable radiation at vacuum ultraviolet wavelengths by using it to excite a rare gas transition at 583.7 A. In addition, this light source was used to make the first measurement of the isotopic shift of the helium metastable level at 601 A. Applications in laser controlled chemistry and spectroscopy, and proposals for new types of lasers using these two energy transfer methods are discussed

Ultrafast Graphene Photonics and Optoelectronics

Science.gov (United States)

2017-04-14

AFRL-AFOSR-JP-TR-2017-0032 Ultrafast Graphene Photonics and Optoelectronics Kuang-Hsiung Wu National Chiao Tung University Final Report 04/14/2017...DATES COVERED (From - To) 18 Apr 2013 to 17 Apr 2016 4. TITLE AND SUBTITLE Ultrafast Graphene Photonics and Optoelectronics 5a.  CONTRACT NUMBER 5b...Prescribed by ANSI Std. Z39.18 Final Report for AOARD Grant FA2386-13-1-4022 “Ultrafast Graphene Photonics and Optoelectronics” Date May 23th, 2016

Ultrafast transmission electron microscopy using a laser-driven field emitter: Femtosecond resolution with a high coherence electron beam

Energy Technology Data Exchange (ETDEWEB)

Feist, Armin; Bach, Nora; Rubiano da Silva, Nara; Danz, Thomas; Möller, Marcel; Priebe, Katharina E.; Domröse, Till; Gatzmann, J. Gregor; Rost, Stefan; Schauss, Jakob; Strauch, Stefanie; Bormann, Reiner; Sivis, Murat; Schäfer, Sascha, E-mail: sascha.schaefer@phys.uni-goettingen.de; Ropers, Claus, E-mail: claus.ropers@uni-goettingen.de

2017-05-15

We present the development of the first ultrafast transmission electron microscope (UTEM) driven by localized photoemission from a field emitter cathode. We describe the implementation of the instrument, the photoemitter concept and the quantitative electron beam parameters achieved. Establishing a new source for ultrafast TEM, the Göttingen UTEM employs nano-localized linear photoemission from a Schottky emitter, which enables operation with freely tunable temporal structure, from continuous wave to femtosecond pulsed mode. Using this emission mechanism, we achieve record pulse properties in ultrafast electron microscopy of 9 Å focused beam diameter, 200 fs pulse duration and 0.6 eV energy width. We illustrate the possibility to conduct ultrafast imaging, diffraction, holography and spectroscopy with this instrument and also discuss opportunities to harness quantum coherent interactions between intense laser fields and free-electron beams. - Highlights: • First implementation of an ultrafast TEM employing a nanoscale photocathode. • Localized single photon-photoemission from nanoscopic field emitter yields low emittance ultrashort electron pulses. • Electron pulses focused down to ~9 Å, with a duration of 200 fs and an energy width of 0.6 eV are demonstrated. • Quantitative characterization of ultrafast electron gun emittance and brightness. • A range of applications of high coherence ultrashort electron pulses is shown.

Ultrafast spectroscopic investigation of a fullerene poly(3-hexylthiophene) dyad

Science.gov (United States)

Banerji, Natalie; Seifter, Jason; Wang, Mingfeng; Vauthey, Eric; Wudl, Fred; Heeger, Alan J.

2011-08-01

We present the femtosecond spectroscopic investigation of a covalently linked dyad, PCB-P3HT, formed by a segment of the conjugated polymer P3HT (regioregular poly(3-hexylthiophene)) that is end capped with the fullerene derivative PCB ([6,6]-phenyl-C61-butyric acid ester), adapted from PCBM. The fluorescence of the P3HT segment in tetrahydrofuran (THF) solution is reduced by 64% in the dyad compared to a control compound without attached fullerene (P3HT-OH). Fluorescence upconversion measurements reveal that the partial fluorescence quenching of PCB-P3HT in THF is multiphasic and occurs on an average time scale of 100 ps, in parallel to excited-state relaxation processes. Judging from ultrafast transient absorption experiments, the origin of the quenching is excitation energy transfer from the P3HT donor to the PCB acceptor. Due to the much higher solubility of P3HT compared to PCB in THF, the PCB-P3HT dyad molecules self-assemble into micelles. When pure C60 is added to the solution, it is incorporated into the fullerene-rich center of the micelles. This dramatically increases the solubility of C60 but does not lead to significant additional quenching of the P3HT fluorescence by the C60 contained in the micelles. In PCB-P3HT thin films drop-cast from THF, the micelle structure is conserved. In contrast to solution, quantitative and ultrafast (microscopy images. Ultrafast charge separation occurs also for the fibrous morphology, but the transient absorption experiments show fast loss of part of the charge carriers due to intensity-induced recombination and annihilation processes and monomolecular interfacial trap-mediated or geminate recombination. The yield of the long-lived charge carriers in the highly organized fibers is however comparable to that obtained with annealed P3HT:PCBM blends. PCB-P3HT can therefore be considered as an active material in organic photovoltaic devices.

Out-and-back {sup 13}C-{sup 13}C scalar transfers in protein resonance assignment by proton-detected solid-state NMR under ultra-fast MAS

Energy Technology Data Exchange (ETDEWEB)

Barbet-Massin, Emeline; Pell, Andrew J. [University of Lyon, CNRS/ENS Lyon/UCB Lyon 1, Centre de RMN a Tres Hauts Champs (France); Jaudzems, Kristaps [Latvian Institute of Organic Synthesis (Latvia); Franks, W. Trent; Retel, Joren S. [Leibniz-Institut fuer Molekulare Pharmakologie (Germany); Kotelovica, Svetlana; Akopjana, Inara; Tars, Kaspars [Biomedical Research and Study Center (Latvia); Emsley, Lyndon [University of Lyon, CNRS/ENS Lyon/UCB Lyon 1, Centre de RMN a Tres Hauts Champs (France); Oschkinat, Hartmut [Leibniz-Institut fuer Molekulare Pharmakologie (Germany); Lesage, Anne; Pintacuda, Guido, E-mail: guido.pintacuda@ens-lyon.fr [University of Lyon, CNRS/ENS Lyon/UCB Lyon 1, Centre de RMN a Tres Hauts Champs (France)

2013-08-15

We present here {sup 1}H-detected triple-resonance H/N/C experiments that incorporate CO-CA and CA-CB out-and-back scalar-transfer blocks optimized for robust resonance assignment in biosolids under ultra-fast magic-angle spinning (MAS). The first experiment, (H)(CO)CA(CO)NH, yields {sup 1}H-detected inter-residue correlations, in which we record the chemical shifts of the CA spins in the first indirect dimension while during the scalar-transfer delays the coherences are present only on the longer-lived CO spins. The second experiment, (H)(CA)CB(CA)NH, correlates the side-chain CB chemical shifts with the NH of the same residue. These high sensitivity experiments are demonstrated on both fully-protonated and 100 %-H{sup N} back-protonated perdeuterated microcrystalline samples of Acinetobacter phage 205 (AP205) capsids at 60 kHz MAS.

Ultrafast Hierarchical OTDM/WDM Network

Directory of Open Access Journals (Sweden)

Hideyuki Sotobayashi

2003-12-01

Full Text Available Ultrafast hierarchical OTDM/WDM network is proposed for the future core-network. We review its enabling technologies: C- and L-wavelength-band generation, OTDM-WDM mutual multiplexing format conversions, and ultrafast OTDM wavelengthband conversions.

Energy transfers in large-scale and small-scale dynamos

Science.gov (United States)

Samtaney, Ravi; Kumar, Rohit; Verma, Mahendra

2015-11-01

We present the energy transfers, mainly energy fluxes and shell-to-shell energy transfers in small-scale dynamo (SSD) and large-scale dynamo (LSD) using numerical simulations of MHD turbulence for Pm = 20 (SSD) and for Pm = 0.2 on 10243 grid. For SSD, we demonstrate that the magnetic energy growth is caused by nonlocal energy transfers from the large-scale or forcing-scale velocity field to small-scale magnetic field. The peak of these energy transfers move towards lower wavenumbers as dynamo evolves, which is the reason for the growth of the magnetic fields at the large scales. The energy transfers U2U (velocity to velocity) and B2B (magnetic to magnetic) are forward and local. For LSD, we show that the magnetic energy growth takes place via energy transfers from large-scale velocity field to large-scale magnetic field. We observe forward U2U and B2B energy flux, similar to SSD.

An abnormally slow proton transfer reaction in a simple HBO derivative due to ultrafast intramolecular-charge transfer events.

Science.gov (United States)

Alarcos, Noemí; Gutierrez, Mario; Liras, Marta; Sánchez, Félix; Douhal, Abderrazzak

2015-07-07

We report on the steady-state, picosecond and femtosecond time-resolved studies of a charge and proton transfer dye 6-amino-2-(2'-hydroxyphenyl)benzoxazole (6A-HBO) and its methylated derivative 6-amino-2-(2'-methoxyphenyl)benzoxazole (6A-MBO), in different solvents. With femtosecond resolution and comparison with the photobehaviour of 6A-MBO, we demonstrate for 6A-HBO in solution, the photoproduction of an intramolecular charge-transfer (ICT) process at S1 taking place in ∼140 fs or shorter, followed by solvent relaxation in the charge transferred species. The generated structure (syn-enol charge transfer conformer) experiences an excited-state intramolecular proton-transfer (ESIPT) reaction to produce a keto-type tautomer. This subsequent proton motion occurs in 1.2 ps (n-heptane), 14 ps (DCM) and 35 ps (MeOH). In MeOH, it is assisted by the solvent molecules and occurs through tunneling for which we got a large kinetic isotope effect (KIE) of about 13. For the 6A-DBO (deuterated sample in CD3OD) the global proton-transfer reaction takes place in 200 ps, showing a remarkable slow KIE regime. The slow ESIPT reaction in DCM (14 ps), not through tunnelling as it is not sensitive to OH/OD exchange, has however to overcome an energy barrier using intramolecular as well as solvent coordinates. The rich ESIPT dynamics of 6A-HBO in the used solutions is governed by an ICT reaction, triggered by the amino group, and it is solvent dependent. Thus, the charge injection to a 6A-HBO molecular frame makes the ICT species more stable, and the phenol group less acidic, slowing down the subsequent ESIPT reaction. Our findings bring new insights into the coupling between ICT and ESIPT reactions on the potential-energy surfaces of several barriers.

Complete elimination of nonlinear light-matter interactions with broadband ultrafast laser pulses

DEFF Research Database (Denmark)

Shu, Chuan-Cun; Dong, Daoyi; Petersen, Ian R.

2017-01-01

optical effects, however, the probability of pure single-photon absorption is usually very low, which is particularly pertinent in the case of strong ultrafast laser pulses with broad bandwidth. Here we demonstrate theoretically a counterintuitive coherent single-photon absorption scheme by eliminating...... nonlinear interactions of ultrafast laser pulses with quantum systems. That is, a completely linear response of the system with respect to the spectral energy density of the incident light at the transition frequency can be obtained for all transition probabilities between 0 and 100% in multilevel quantum...... systems. To that end, a multiobjective optimization algorithm is developed to find an optimal spectral phase of an ultrafast laser pulse, which is capable of eliminating all possible nonlinear optical responses while maximizing the probability of single-photon absorption between quantum states. This work...

Visual prosthesis wireless energy transfer system optimal modeling.

Science.gov (United States)

Li, Xueping; Yang, Yuan; Gao, Yong

2014-01-16

Wireless energy transfer system is an effective way to solve the visual prosthesis energy supply problems, theoretical modeling of the system is the prerequisite to do optimal energy transfer system design. On the basis of the ideal model of the wireless energy transfer system, according to visual prosthesis application condition, the system modeling is optimized. During the optimal modeling, taking planar spiral coils as the coupling devices between energy transmitter and receiver, the effect of the parasitic capacitance of the transfer coil is considered, and especially the concept of biological capacitance is proposed to consider the influence of biological tissue on the energy transfer efficiency, resulting in the optimal modeling's more accuracy for the actual application. The simulation data of the optimal model in this paper is compared with that of the previous ideal model, the results show that under high frequency condition, the parasitic capacitance of inductance and biological capacitance considered in the optimal model could have great impact on the wireless energy transfer system. The further comparison with the experimental data verifies the validity and accuracy of the optimal model proposed in this paper. The optimal model proposed in this paper has a higher theoretical guiding significance for the wireless energy transfer system's further research, and provide a more precise model reference for solving the power supply problem in visual prosthesis clinical application.

Photoinduced intermolecular electron transfer and off-resonance Raman characteristics of Rhodamine 101/N,N-diethylaniline

International Nuclear Information System (INIS)

Jiang, Li-lin; Liu, Wei-long; Song, Yun-fei; He, Xing; Wang, Yang; Wang, Chang; Wu, Hong-lin; Yang, Fang; Yang, Yan-qiang

2014-01-01

Highlights: • Mechanism of PIET reaction process for the Rh101 + /DEA system is investigated. • The significant geometrical changes of the charge–transfer complex are explained. • Forward Electron transfer from DEA to Rh101 +∗ occurs with lifetime of 425–560 fs. • Backward electron transfer occurs with a time constant of 46.16–51.40 ps. • Intramolecular vibrational relaxation occurs with lifetime of 2.77–5.39 ps. - Abstract: The ultrafast photoinduced intermolecular electron transfer (PIET) reaction of Rhodamine 101 (Rh101 + ) in N,N-diethylaniline (DEA) was investigated using off-resonance Raman, femtosecond time-resolved multiplex transient grating (TG) and transient absorption (TA) spectroscopies. The Raman spectra indicate that the C=C stretching vibration of the chromophore aromatic ring is more sensitive to ET compared with the C-C stretching mode. The ultrafast photoinduced intermolecular forward ET (FET) from DEA to Rh101 +∗ occurs on a time scale of τ FET = 425–560 fs. The backward ET (BET) occurs in the inverted region with a time constant of τ BET = 46.16–51.40 ps. The intramolecular vibrational relaxation (IVR) process occurs on the excited state potential energy surface with the time constant of τ IVR = 2.77–5.39 ps

The security energy encryption in wireless power transfer

Science.gov (United States)

Sadzali, M. N.; Ali, A.; Azizan, M. M.; Albreem, M. A. M.

2017-09-01

This paper presents a concept of security in wireless power transfer (WPT) by applying chaos theory. Chaos theory is applied as a security system in order to safeguard the transfer of energy from a transmitter to the intended receiver. The energy encryption of the wireless power transfer utilizes chaos theory to generate the possibility of a logistic map for the chaotic security key. The simulation for energy encryption wireless power transfer system was conducted by using MATLAB and Simulink. By employing chaos theory, the chaotic key ensures the transmission of energy from transmitter to its intended receiver.

Avant-Garde Ultrafast Laser Writing

Directory of Open Access Journals (Sweden)

Kazansky P. G.

2013-11-01

Full Text Available Ultrafast laser processing of transparent materials reveals new phenomena. Reviewed, are recent demonstrations of 5D optical memory, vortex polarization and Airy beam converters employing self-assembled nanostructuring, ultrafast laser calligraphy and polarization writing control using pulses with tilted front.

Ultrafast Photovoltaic Response in Ferroelectric Nanolayers

Science.gov (United States)

2016-04-19

the free energy of the system [3,4,8]. Intensive research has been aimed at bypassing the intrinsic size limits imposed by the depolarization field...Page 1 of 21   Ultrafast photovoltaic response in ferroelectric nanolayers Dan Daranciang1,2, Matthew J. Highland3, Haidan Wen4, Steve M. Young5...ferroelectric PbTiO3 via direct coupling to its intrinsic photovoltaic response. Using time-resolved x-ray scattering to visualize atomic displacements on

Ultrafast nonlinear optics

CERN Document Server

Leburn, Christopher; Reid, Derryck

2013-01-01

The field of ultrafast nonlinear optics is broad and multidisciplinary, and encompasses areas concerned with both the generation and measurement of ultrashort pulses of light, as well as those concerned with the applications of such pulses. Ultrashort pulses are extreme events – both in terms of their durations, and also the high peak powers which their short durations can facilitate. These extreme properties make them powerful experiment tools. On one hand, their ultrashort durations facilitate the probing and manipulation of matter on incredibly short timescales. On the other, their ultrashort durations can facilitate high peak powers which can drive highly nonlinear light-matter interaction processes. Ultrafast Nonlinear Optics covers a complete range of topics, both applied and fundamental in nature, within the area of ultrafast nonlinear optics. Chapters 1 to 4 are concerned with the generation and measurement of ultrashort pulses. Chapters 5 to 7 are concerned with fundamental applications of ultrasho...

rf streak camera based ultrafast relativistic electron diffraction.

Science.gov (United States)

Musumeci, P; Moody, J T; Scoby, C M; Gutierrez, M S; Tran, T

2009-01-01

We theoretically and experimentally investigate the possibility of using a rf streak camera to time resolve in a single shot structural changes at the sub-100 fs time scale via relativistic electron diffraction. We experimentally tested this novel concept at the UCLA Pegasus rf photoinjector. Time-resolved diffraction patterns from thin Al foil are recorded. Averaging over 50 shots is required in order to get statistics sufficient to uncover a variation in time of the diffraction patterns. In the absence of an external pump laser, this is explained as due to the energy chirp on the beam out of the electron gun. With further improvements to the electron source, rf streak camera based ultrafast electron diffraction has the potential to yield truly single shot measurements of ultrafast processes.

Interactive Joint Transfer of Energy and Information

DEFF Research Database (Denmark)

Popovski, Petar; Fouladgar, A. M.; Simeone, Osvaldo

2013-01-01

In some communication networks, such as passive RFID systems, the energy used to transfer information between a sender and a recipient can be reused for successive communication tasks. In fact, from known results in physics, any system that exchanges information via the transfer of given physical...... key design insights. Index Terms— Two-way channel, interactive communication, energy transfer, energy harvesting....... resources, such as radio waves, particles and qubits, can conceivably reuse, at least part, of the received resources. This paper aims at illustrating some of the new challenges that arise in the design of communication networks in which the signals exchanged by the nodes carry both information and energy...

Ultrafast electron injection at the cationic porphyrin-graphene interface assisted by molecular flattening

KAUST Repository

Aly, Shawkat Mohammede; Parida, Manas R.; Alarousu, Erkki; Mohammed, Omar F.

2014-01-01

The steady-state and femtosecond (fs) time-resolved data clearly demonstrate that the charge transfer (CT) process at the porphyrin-graphene carboxylate (GC) interfaces can be tuned from zero to very sufficient and ultrafast by changing the electronic structure of the meso unit and the redox properties of the porphyrin cavity. This journal is © the Partner Organisations 2014.

Ultrafast transient-absorption of the solvated electron in water

International Nuclear Information System (INIS)

Kimura, Y.; Alfano, J.C.; Walhout, P.K.; Barbara, P.F.

1994-01-01

Ultrafast near infrared (NIR)-pump/variable wavelength probe transient-absorption spectroscopy has been performed on the aqueous solvated electron. The photodynamics of the solvated electron excited to its p-state are qualitatively similar to previous measurements of the dynamics of photoinjected electrons at high energy. This result confirms the previous interpretation of photoinjected electron dynamics as having a rate-limiting bottleneck at low energies presumably involving the p-state

A planning framework for transferring building energy technologies

Energy Technology Data Exchange (ETDEWEB)

Farhar, B C; Brown, M A; Mohler, B L; Wilde, M; Abel, F H

1990-07-01

Accelerating the adoption of new and existing cost-effective technologies has significant potential to reduce the energy consumed in US buildings. This report presents key results of an interlaboratory technology transfer planning effort in support of the US Department of Energy's Office of Building Technologies (OBT). A guiding assumption for planning was that OBT's R D program should forge linkages with existing programs whose goals involved enhancing energy efficiency in buildings. An ad hoc Technology Transfer Advisory Group reviewed the existing analysis and technology transfer program, brainstormed technology transfer approaches, interviewed DOE program managers, identified applicable research results, and developed a framework that management could use in deciding on the best investments of technology transfer resources. Representatives of 22 organizations were interviewed on their views of the potential for transferring energy efficiency technologies through active linking with OBT. The report describes these programs and interview results; outlines OBT tools, technologies, and practices to be transferred; defines OBT audiences; identifies technology transfer functions and presents a framework devised using functions and audiences; presents some 60 example technology transfer activities; and documents the Advisory Group's recommendations. 37 refs., 3 figs., 12 tabs.

Ultrafast dynamics of correlated electrons

International Nuclear Information System (INIS)

Rettig, Laurenz

2012-01-01

This work investigates the ultrafast electron dynamics in correlated, low-dimensional model systems using femtosecond time- and angle-resolved photoemission spectroscopy (trARPES) directly in the time domain. In such materials, the strong electron-electron (e-e) correlations or coupling to other degrees of freedom such as phonons within the complex many-body quantum system lead to new, emergent properties that are characterized by phase transitions into broken-symmetry ground states such as magnetic, superconducting or charge density wave (CDW) phases. The dynamical processes related to order like transient phase changes, collective excitations or the energy relaxation within the system allow deeper insight into the complex physics governing the emergence of the broken-symmetry state. In this work, several model systems for broken-symmetry ground states and for the dynamical charge balance at interfaces have been studied. In the quantum well state (QWS) model system Pb/Si(111), the charge transfer across the Pb/Si interface leads to an ultrafast energetic stabilization of occupied QWSs, which is the result of an increase of the electronic confinement to the metal film. In addition, a coherently excited surface phonon mode is observed. In antiferromagnetic (AFM) Fe pnictide compounds, a strong momentum-dependent asymmetry of electron and hole relaxation rates allows to separate the recovery dynamics of the AFM phase from electron-phonon (e-ph) relaxation. The strong modulation of the chemical potential by coherent phonon modes demonstrates the importance of e-ph coupling in these materials. However, the average e-ph coupling constant is found to be small. The investigation of the excited quasiparticle (QP) relaxation dynamics in the high-T c 4 superconductor Bi 2 Sr 2 CaCu 2 O 8+δ reveals a striking momentum and fluence independence of the QP life times. In combination with the momentum-dependent density of excited QPs, this demonstrates the suppression of momentum

Intermolecular energy transfer in binary systems of dye polymers

Science.gov (United States)

Liu, Lin-I.; Barashkov, Nikolay N.; Palsule, Chintamani P.; Gangopadhyay, Shubhra; Borst, Walter L.

2000-10-01

We present results and physical interpretations for the energy transfer mechanisms in two-component dye polymer systems. The data consist of fluorescence emission spectra and decays. Two dyes were embedded in an epoxypolymer base, and only they participated in the energy transfer. Following pulsed laser excitation of the donor dye, energy transfer took place to the accept dye. The possible transfer paths considered here were nonradiative and radiative transfer. The latter involves two steps, emission and absorption of a photon, and therefore is relatively slow, while nonradiative transfer is a fast single step resulting from direct Coulomb interactions. A predominantly nonradiative transfer is desirable for applications, for instance in wavelength shifters in high energy particle detection. We studied the concentration effects of the dyes on the energy transfer and obtained the relative quantum efficiencies of various wavelength shifters from the fluorescence emission spectra. For low acceptor concentrations, radiative transfer was found to dominate, while nonradiative transfer became dominant at increasing dye concentrations. The fluorescence decays were analyzed with a sum-of-exponentials method and with Förster kinetics. The sum of exponential model yielded mean decay times of the dye polymers useful for a general classification. The decay times decreased as desired with increasing acceptor concentration. The samples, in which nonradiative energy transfer dominated, were analyzed with Förster kinetics. As a result, the natural decay times of the donor and acceptor dyes and the critical radii for nonradiative energy transfer were obtained from a global best fit.

Ultrafast carrier dynamics in band edge and broad deep defect emission ZnSe nanowires

Science.gov (United States)

Othonos, Andreas; Lioudakis, Emmanouil; Philipose, U.; Ruda, Harry E.

2007-12-01

Ultrafast carrier dynamics of ZnSe nanowires grown under different growth conditions have been studied. Transient absorption measurements reveal the dependence of the competing effects of state filling and photoinduced absorption on the probed energy states. The relaxation of the photogenerated carriers occupying defect states in the stoichiometric and Se-rich samples are single exponentials with time constants of 3-4ps. State filling is the main contribution for probe energies below 1.85eV in the Zn-rich grown sample. This ultrafast carrier dynamics study provides an important insight into the role that intrinsic point defects play in the observed photoluminescence from ZnSe nanowires.

Research on the ultrafast fluorescence property of thylakoid membranes of the wild-type and mutant rice

Science.gov (United States)

Ren, Zhao-Yu; Xu, Xiao-Ming; Wang, Shui-Cai; Xin, Yue-Yong; He, Jun-Fang; Hou, Xun

2003-10-01

A high yielding rice variety mutant (Oryza sativa L., Zhenhui 249) with low chlorophyll b (Chl b) has been discovered in natural fields. It has a quality character controlled by a pair of recessive genes (nuclear gene). The partial loss of Chl b in content affects the efficiency of light harvest in a light harvest complex (LHC), thus producing the difference of the exciting energy transfer and the efficiency of photochemistry conversion between the mutant and wild-type rice in photosynthetic unit. The efficiency of utilizing light energy is higher in the mutant than that in the wild-type rice relatively. For further discussion of the above-mentioned difference and learning about the mechanism of the increase in the photochemical efficiency of the mutant, the pico-second resolution fluorescence spectrum measurement with delay-frame-scanning single photon counting technique is adopted. Thylakoid membranes of the mutant and the wild-type rice are excited by an Ar+ laser with a pulse width of 120 ps, repetition rate of 4 MHz and wavelength of 514 nm. Compared with the time and spectrum property of exciting fluorescence, conclusions of those ultrafast dynamic experiments are: 1) The speeds of the exciting energy transferred in photo-system I are faster than that in photo-system II in both samples. 2) The speeds of the exciting energy transfer of mutant sample are faster than those of the wild-type. This might be one of the major reasons why the efficiency of photosynthesis is higher in mutant than that in the wild-type rice.

Energy transfer mechanism between manganese and neodymium

Energy Technology Data Exchange (ETDEWEB)

Kumar, R [Department of Physics, Government Raza Post-Graduate College, Rampur 244901, U.P., India

1977-01-01

The mechanism of energy transfer between Mn/sup 2 +/ ..-->.. Nd/sup 3 +/ in barium borate glass has been investigated. The change in emission intensities and lifetimes of Mn/sup 2 +/ (donor) due to the presence of Nd/sup 3 +/ (acceptor) are observed. It has been concluded that the mechanism of energy transfer involves a nonradiative resonance process. The electrostatic multiple interaction responsible for the transfer is dipole-dipole in nature.

DeepNet: An Ultrafast Neural Learning Code for Seismic Imaging

International Nuclear Information System (INIS)

Barhen, J.; Protopopescu, V.; Reister, D.

1999-01-01

A feed-forward multilayer neural net is trained to learn the correspondence between seismic data and well logs. The introduction of a virtual input layer, connected to the nominal input layer through a special nonlinear transfer function, enables ultrafast (single iteration), near-optimal training of the net using numerical algebraic techniques. A unique computer code, named DeepNet, has been developed, that has achieved, in actual field demonstrations, results unattainable to date with industry standard tools

Resonance energy transfer: Dye to metal nanoparticles

Energy Technology Data Exchange (ETDEWEB)

Wari, M. N.; Pujar, G. H.; Inamdar, S. R., E-mail: him-lax3@yahoo.com [Laser Spectroscopy Programme, Department of Physics, Karnatak University, Dharwad-580003 (India)

2015-06-24

In the present study, surface energy transfer (SET) from Coumarin 540A (C540 A) to Gold nanoparticle (Au) is demonstrated. The observed results show pronounced effect on the photoluminescence intensity and shortening of the lifetime of Coumarin 540A upon interaction with the spherical gold nanoparticle, also there are measured effects on radiative rate of the dye. Experimental results are analyzed with fluorescence resonance energy transfer (FRET) and SET theories. The results obtained from distance-dependent quenching provide experimental evidence that the efficiency curve slope and distance of quenching is best modeled by surface energy transfer process.

Risk transfer via energy savings insurance

Energy Technology Data Exchange (ETDEWEB)

Mills, Evan

2001-10-01

Among the key barriers to investment in energy efficiency improvements are uncertainties about attaining projected energy savings and apprehension about potential disputes over these savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building commissioning), financial risk transfer techniques are less developed in the energy management arena than in other more mature segments of the economy. Energy Savings Insurance (ESI) - formal insurance of predicted energy savings - is one method of transferring financial risks away from the facility owner or energy services contractor. ESI offers a number of significant advantages over other forms of financial risk transfer, e.g. savings guarantees or performance bonds. ESI providers manage risk via pre-construction design review as well as post-construction commissioning and measurement and verification of savings. We found that the two mos t common criticisms of ESI - excessive pricing and onerous exclusions - are not born out in practice. In fact, if properly applied, ESI can potentially reduce the net cost of energy savings projects by reducing the interest rates charged by lenders, and by increasing the level of savings through quality control. Debt service can also be ensured by matching loan payments to projected energy savings while designing the insurance mechanism so that payments are made by the insurer in the event of a savings shortfall. We estimate the U.S. ESI market potential of $875 million/year in premium income. From an energy-policy perspective, ESI offers a number of potential benefits: ESI transfers performance risk from the balance sheet of the entity implementing the energy savings project, thereby freeing up capital otherwise needed to ''self-insure'' the savings. ESI reduces barriers to market entry of smaller energy services firms who do not have sufficiently strong balance

Energy transfer during the hydroentanglement of fibres

CSIR Research Space (South Africa)

Moyo, D

2012-10-01

Full Text Available .kashan.co.za] ABSTRACT The hydroentanglement of fibres is achieved by the energy of the high-velocity waterjets. This method is highly energy intensive and costly, hence the attempt to study the energy transfer during the process. Generally, the amount of energy used... in the nonwoven fabric strength were studied. In the study, the energies of the waterjets transferred to every fabric sample as a function of the waterjet pressure, machine speed, machine efficiency and the web area weight were quantified, and the resultant...

Resonant vibrational energy transfer in ice Ih

Energy Technology Data Exchange (ETDEWEB)

Shi, L.; Li, F.; Skinner, J. L. [Theoretical Chemistry Institute and Department of Chemistry, University of Wisconsin, Madison, Wisconsin 53706 (United States)

2014-06-28

Fascinating anisotropy decay experiments have recently been performed on H{sub 2}O ice Ih by Timmer and Bakker [R. L. A. Timmer, and H. J. Bakker, J. Phys. Chem. A 114, 4148 (2010)]. The very fast decay (on the order of 100 fs) is indicative of resonant energy transfer between OH stretches on different molecules. Isotope dilution experiments with deuterium show a dramatic dependence on the hydrogen mole fraction, which confirms the energy transfer picture. Timmer and Bakker have interpreted the experiments with a Förster incoherent hopping model, finding that energy transfer within the first solvation shell dominates the relaxation process. We have developed a microscopic theory of vibrational spectroscopy of water and ice, and herein we use this theory to calculate the anisotropy decay in ice as a function of hydrogen mole fraction. We obtain very good agreement with experiment. Interpretation of our results shows that four nearest-neighbor acceptors dominate the energy transfer, and that while the incoherent hopping picture is qualitatively correct, vibrational energy transport is partially coherent on the relevant timescale.

Pumped energy transfer stations (STEP)

International Nuclear Information System (INIS)

Tournery, Jean-Francois

2015-12-01

As objectives of development are high for renewable energies (they are supposed to cover 50 per cent of new energy needs by 2035), pumped energy transfer stations are to play an important role in this respect. The author first discusses the consequences of the development of renewable energies on the exploitation of electric grids: issue of intermittency for some of them, envisaged solutions. Then, he addresses one of the solutions: the storage of electric power. He notices that increasing the potential energy of a volume of water is presently the most mature solution to face massive needs of the power system. Dams and pumped energy transfer stations represent now almost the whole installed storage power in the world. The author then presents these pumped energy transfer stations: principle, brief history (the first appeared in Italy and Switzerland at the end of the 1890's). He indicates the various parameters of assessment of such stations: maximum stored energy, installed power in pumping mode and turbine mode, time constant, efficiency, level of flexibility. He discusses economic issues. He describes and comments the operation of turbine-pump groups: ternary groups, reversible binary groups. He discusses barriers to be overcome and technical advances to be made for varying speed groups and for marine stations. He finally gives an overview (table with number of stations belonging to different power ranges, remarkable installations) of existing stations in China, USA, Japan, Germany, Austria, Spain, Portugal, Italy, Switzerland, France and UK, and indicate predictions regarding storage needs at the world level. Some data are finally indicated for the six existing French installations

Electromagnetic Energy Absorption due to Wireless Energy Transfer: A Brief Review

Directory of Open Access Journals (Sweden)

Syafiq A.

2016-01-01

Full Text Available This paper reviews an implementation of evaluating compliance of wireless power transfer systems with respect to human electromagnetic exposure limits. Methods for both numerical analysis and measurements are discussed. The objective is to evaluate the rate of which energy is absorbed by the human body when exposed to a wireless energy transfer, although it can be referred to the absorption of other forms of energy by tissue. An exposure assessment of a representative wireless power transfer system, under a limited set of operating conditions, is provided in order to estimate the maximum SAR levels. The aim of this review is to conclude the possible side effect to the human body when utilizing wireless charging in daily life so that an early severe action can be taken when using wireless transfer.

Integrated analysis of energy transfers in elastic-wave turbulence.

Science.gov (United States)

Yokoyama, Naoto; Takaoka, Masanori

2017-08-01

In elastic-wave turbulence, strong turbulence appears in small wave numbers while weak turbulence does in large wave numbers. Energy transfers in the coexistence of these turbulent states are numerically investigated in both the Fourier space and the real space. An analytical expression of a detailed energy balance reveals from which mode to which mode energy is transferred in the triad interaction. Stretching energy excited by external force is transferred nonlocally and intermittently to large wave numbers as the kinetic energy in the strong turbulence. In the weak turbulence, the resonant interactions according to the weak turbulence theory produce cascading net energy transfer to large wave numbers. Because the system's nonlinearity shows strong temporal intermittency, the energy transfers are investigated at active and moderate phases separately. The nonlocal interactions in the Fourier space are characterized by the intermittent bundles of fibrous structures in the real space.

Heat transfer between adsorbate and laser-heated hot electrons

International Nuclear Information System (INIS)

Ueba, H; Persson, B N J

2008-01-01

Strong short laser pulses can give rise to a strong increase in the electronic temperature at metal surfaces. Energy transfer from the hot electrons to adsorbed molecules may result in adsorbate reactions, e.g. desorption or diffusion. We point out the limitations of an often used equation to describe the heat transfer process in terms of a friction coupling. We propose a simple theory for the energy transfer between the adsorbate and hot electrons using a newly introduced heat transfer coefficient, which depends on the adsorbate temperature. We calculate the transient adsorbate temperature and the reaction yield for a Morse potential as a function of the laser fluency. The results are compared to those obtained using a conventional heat transfer equation with temperature-independent friction. It is found that our equation of energy (heat) transfer gives a significantly lower adsorbate peak temperature, which results in a large modification of the reaction yield. We also consider the heat transfer between different vibrational modes excited by hot electrons. This mode coupling provides indirect heating of the vibrational temperature in addition to the direct heating by hot electrons. The formula of heat transfer through linear mode-mode coupling of two harmonic oscillators is applied to the recent time-resolved study of carbon monoxide and atomic oxygen hopping on an ultrafast laser-heated Pt(111) surface. It is found that the maximum temperature of the frustrated translation mode can reach high temperatures for hopping, even when direct friction coupling to the hot electrons is not strong enough

Plasmonic energy transfer in periodically doped graphene

International Nuclear Information System (INIS)

Silveiro, I; Manjavacas, A; Thongrattanasiri, S; García de Abajo, F J

2013-01-01

We predict unprecedentedly large values of the energy-transfer rate between an optical emitter and a layer of periodically doped graphene. The transfer exhibits divergences at photon frequencies corresponding to the Van Hove singularities of the plasmonic band structure of the graphene. In particular, we find flat bands associated with regions of vanishing doping charge, which appear in graphene when it is patterned through gates of spatially alternating signs, giving rise to intense transfer rate singularities. Graphene is thus shown to provide a unique platform for fast control of optical energy transfer via fast electrostatic inhomogeneous doping. (paper)

Ultrafast THz saturable absorption in doped semiconductors at room temperature

DEFF Research Database (Denmark)

Turchinovich, Dmitry; Hoffmann, M. V.

2011-01-01

Ultrafast Phenomena XVII presents the latest advances in ultrafast science, including both ultrafast optical technology and the study of ultrafast phenomena. It covers picosecond, femtosecond and attosecond processes relevant to applications in physics, chemistry, biology, and engineering. Ultraf...

The Grover energy transfer algorithm for relativistic speeds

International Nuclear Information System (INIS)

Garcia-Escartin, Juan Carlos; Chamorro-Posada, Pedro

2010-01-01

Grover's algorithm for quantum search can also be applied to classical energy transfer. The procedure takes a system in which the total energy is equally distributed among N subsystems and transfers most of it to one marked subsystem. We show that in a relativistic setting the efficiency of this procedure can be improved. We will consider the transfer of relativistic kinetic energy in a series of elastic collisions. In this case, the number of steps of the energy transfer procedure approaches 1 as the initial velocities of the objects become closer to the speed of light. This is a consequence of introducing nonlinearities in the procedure. However, the maximum attainable transfer will depend on the particular combination of speed and number of objects. In the procedure, we will use N elements, as in the classical non-relativistic case, instead of the log 2 (N) states of the quantum algorithm.

Optical Energy Transfer and Conversion System

Science.gov (United States)

Hogan, Bartholomew P. (Inventor); Stone, William C. (Inventor)

2018-01-01

An optical energy transfer and conversion system comprising a fiber spooler and an electrical power extraction subsystem connected to the spooler with an optical waveguide. Optical energy is generated at and transferred from a base station through fiber wrapped around the spooler, and ultimately to the power extraction system at a remote mobility platform for conversion to another form of energy. The fiber spooler may reside on the remote mobility platform which may be a vehicle, or apparatus that is either self-propelled or is carried by a secondary mobility platform either on land, under the sea, in the air or in space.

Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode

Energy Technology Data Exchange (ETDEWEB)

Bücker, K.; Picher, M.; Crégut, O. [Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess, 67034 Strasbourg (France); LaGrange, T. [Interdisciplinary Centre for Electron Microscopy, École Polytechnique Fédérale de Lausanne, 1015 Lausanne (Switzerland); Reed, B.W.; Park, S.T.; Masiel, D.J. [Integrated Dynamic Electron Solutions, Inc., 5653 Stoneridge Drive 117, Pleasanton, CA 94588 (United States); Banhart, F., E-mail: florian.banhart@ipcms.unistra.fr [Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess, 67034 Strasbourg (France)

2016-12-15

High temporal resolution transmission electron microscopy techniques have shown significant progress in recent years. Using photoelectron pulses induced by ultrashort laser pulses on the cathode, these methods can probe ultrafast materials processes and have revealed numerous dynamic phenomena at the nanoscale. Most recently, the technique has been implemented in standard thermionic electron microscopes that provide a flexible platform for studying material's dynamics over a wide range of spatial and temporal scales. In this study, the electron pulses in such an ultrafast transmission electron microscope are characterized in detail. The microscope is based on a thermionic gun with a Wehnelt electrode and is operated in a stroboscopic photoelectron mode. It is shown that the Wehnelt bias has a decisive influence on the temporal and energy spread of the picosecond electron pulses. Depending on the shape of the cathode and the cathode-Wehnelt distance, different emission patterns with different pulse parameters are obtained. The energy spread of the pulses is determined by space charge and Boersch effects, given by the number of electrons in a pulse. However, filtering effects due to the chromatic aberrations of the Wehnelt electrode allow the extraction of pulses with narrow energy spreads. The temporal spread is governed by electron trajectories of different length and in different electrostatic potentials. High temporal resolution is obtained by excluding shank emission from the cathode and aberration-induced halos in the emission pattern. By varying the cathode-Wehnelt gap, the Wehnelt bias, and the number of photoelectrons in a pulse, tradeoffs between energy and temporal resolution as well as beam intensity can be made as needed for experiments. Based on the characterization of the electron pulses, the optimal conditions for the operation of ultrafast TEMs with thermionic gun assembly are elaborated. - Highlights: • A detailed characterization of electron

Power scaling of ultrafast mid-IR source enabled by high-power fiber laser technology

Energy Technology Data Exchange (ETDEWEB)

Zhou, Gengji

2017-11-15

Ultrafast laser sources with high repetition-rate (>10 MHz) and tunable in the mid-infrared (IR) wavelength range of 7-18 μm hold promise for many important spectroscopy applications. Currently, these ultrafast mid- to longwavelength-IR sources can most easily be achieved via difference-frequency generation (DFG) between a pump beam and a signal beam. However, current ultrafast mid- to longwavelength-IR sources feature a low average power, which limits their applications. In this thesis, we propose and demonstrate a novel approach to power scaling of DFG-based ultrafast mid-IR laser sources. The essence of this novel approach is the generation of a high-energy signal beam. Both the pump beam and the signal beam are derived from a home-built Yb-fiber laser system that emits 165-fs pulses centered at 1035 nm with 30-MHz repetition rate and 14.5-W average power (corresponding to 483-nJ pulse energy). We employ fiber-optic self-phase modulation (SPM) to broaden the laser spectrum and generate isolated spectral lobes. Filtering the rightmost spectral lobe leads to femtosecond pulses with >10 nJ pulse energy. Tunable between 1.1-1.2 μm, this SPM-enabled ultrafast source exhibits ∝100 times higher pulse energy than can be obtained from Raman soliton sources in this wavelength range. We use this SPM-enabled source as the signal beam and part of the Yb-fiber laser output as the pump beam. By performing DFG in GaSe crystals, we demonstrate that power scaling of a DFG-based mid-IR source can be efficiently achieved by increasing the signal energy. The resulting mid-IR source is tunable from 7.4 μm to 16.8 μm. Up to 5.04-mW mid-IR pulses centered at 11 μm are achieved. The corresponding pulse energy is 167 pJ, representing nearly one order of magnitude improvement compared with other reported DFG-based mid-IR sources at this wavelength. Despite of low pulse energy, Raman soliton sources have become a popular choice as the signal source. We carry out a detailed study on

Power scaling of ultrafast mid-IR source enabled by high-power fiber laser technology

International Nuclear Information System (INIS)

Zhou, Gengji

2017-11-01

Ultrafast laser sources with high repetition-rate (>10 MHz) and tunable in the mid-infrared (IR) wavelength range of 7-18 μm hold promise for many important spectroscopy applications. Currently, these ultrafast mid- to longwavelength-IR sources can most easily be achieved via difference-frequency generation (DFG) between a pump beam and a signal beam. However, current ultrafast mid- to longwavelength-IR sources feature a low average power, which limits their applications. In this thesis, we propose and demonstrate a novel approach to power scaling of DFG-based ultrafast mid-IR laser sources. The essence of this novel approach is the generation of a high-energy signal beam. Both the pump beam and the signal beam are derived from a home-built Yb-fiber laser system that emits 165-fs pulses centered at 1035 nm with 30-MHz repetition rate and 14.5-W average power (corresponding to 483-nJ pulse energy). We employ fiber-optic self-phase modulation (SPM) to broaden the laser spectrum and generate isolated spectral lobes. Filtering the rightmost spectral lobe leads to femtosecond pulses with >10 nJ pulse energy. Tunable between 1.1-1.2 μm, this SPM-enabled ultrafast source exhibits ∝100 times higher pulse energy than can be obtained from Raman soliton sources in this wavelength range. We use this SPM-enabled source as the signal beam and part of the Yb-fiber laser output as the pump beam. By performing DFG in GaSe crystals, we demonstrate that power scaling of a DFG-based mid-IR source can be efficiently achieved by increasing the signal energy. The resulting mid-IR source is tunable from 7.4 μm to 16.8 μm. Up to 5.04-mW mid-IR pulses centered at 11 μm are achieved. The corresponding pulse energy is 167 pJ, representing nearly one order of magnitude improvement compared with other reported DFG-based mid-IR sources at this wavelength. Despite of low pulse energy, Raman soliton sources have become a popular choice as the signal source. We carry out a detailed study on

Ultrafast Laser-Based Spectroscopy and Sensing: Applications in LIBS, CARS, and THz Spectroscopy

Science.gov (United States)

Leahy-Hoppa, Megan R.; Miragliotta, Joseph; Osiander, Robert; Burnett, Jennifer; Dikmelik, Yamac; McEnnis, Caroline; Spicer, James B.

2010-01-01

Ultrafast pulsed lasers find application in a range of spectroscopy and sensing techniques including laser induced breakdown spectroscopy (LIBS), coherent Raman spectroscopy, and terahertz (THz) spectroscopy. Whether based on absorption or emission processes, the characteristics of these techniques are heavily influenced by the use of ultrafast pulses in the signal generation process. Depending on the energy of the pulses used, the essential laser interaction process can primarily involve lattice vibrations, molecular rotations, or a combination of excited states produced by laser heating. While some of these techniques are currently confined to sensing at close ranges, others can be implemented for remote spectroscopic sensing owing principally to the laser pulse duration. We present a review of ultrafast laser-based spectroscopy techniques and discuss the use of these techniques to current and potential chemical and environmental sensing applications. PMID:22399883

Ultrafast Laser-Based Spectroscopy and Sensing: Applications in LIBS, CARS, and THz Spectroscopy

Directory of Open Access Journals (Sweden)

Megan R. Leahy-Hoppa

2010-04-01

Full Text Available Ultrafast pulsed lasers find application in a range of spectroscopy and sensing techniques including laser induced breakdown spectroscopy (LIBS, coherent Raman spectroscopy, and terahertz (THz spectroscopy. Whether based on absorption or emission processes, the characteristics of these techniques are heavily influenced by the use of ultrafast pulses in the signal generation process. Depending on the energy of the pulses used, the essential laser interaction process can primarily involve lattice vibrations, molecular rotations, or a combination of excited states produced by laser heating. While some of these techniques are currently confined to sensing at close ranges, others can be implemented for remote spectroscopic sensing owing principally to the laser pulse duration. We present a review of ultrafast laser-based spectroscopy techniques and discuss the use of these techniques to current and potential chemical and environmental sensing applications.

Photoinduced intermolecular electron transfer and off-resonance Raman characteristics of Rhodamine 101/N,N-diethylaniline

Energy Technology Data Exchange (ETDEWEB)

Jiang, Li-lin [Department of Physics, Harbin Institute of Technology, Harbin 150001 (China); School of Mechanical and Electronic Engineering, Hezhou University, Hezhou 542800 (China); Liu, Wei-long; Song, Yun-fei; He, Xing; Wang, Yang; Wang, Chang; Wu, Hong-lin [Department of Physics, Harbin Institute of Technology, Harbin 150001 (China); Yang, Fang [National Key Laboratory of Science and Technology on Tunable Laser, Department of Optoelectronics Information Science Technology, Harbin Institute of Technology, Harbin 150001 (China); Yang, Yan-qiang, E-mail: yqyang@hit.edu.cn [Department of Physics, Harbin Institute of Technology, Harbin 150001 (China); National Key Laboratory of Shock Wave and Detonation Physics, Institute of Fluid Physics, China Academy of Engineering Physics, Mianyang 621900, Sichuan (China)

2014-01-31

Highlights: • Mechanism of PIET reaction process for the Rh101{sup +}/DEA system is investigated. • The significant geometrical changes of the charge–transfer complex are explained. • Forward Electron transfer from DEA to Rh101{sup +∗} occurs with lifetime of 425–560 fs. • Backward electron transfer occurs with a time constant of 46.16–51.40 ps. • Intramolecular vibrational relaxation occurs with lifetime of 2.77–5.39 ps. - Abstract: The ultrafast photoinduced intermolecular electron transfer (PIET) reaction of Rhodamine 101 (Rh101{sup +}) in N,N-diethylaniline (DEA) was investigated using off-resonance Raman, femtosecond time-resolved multiplex transient grating (TG) and transient absorption (TA) spectroscopies. The Raman spectra indicate that the C=C stretching vibration of the chromophore aromatic ring is more sensitive to ET compared with the C-C stretching mode. The ultrafast photoinduced intermolecular forward ET (FET) from DEA to Rh101{sup +∗} occurs on a time scale of τ{sub FET} = 425–560 fs. The backward ET (BET) occurs in the inverted region with a time constant of τ{sub BET} = 46.16–51.40 ps. The intramolecular vibrational relaxation (IVR) process occurs on the excited state potential energy surface with the time constant of τ{sub IVR} = 2.77–5.39 ps.

The Grover energy transfer algorithm for relativistic speeds

Energy Technology Data Exchange (ETDEWEB)

Garcia-Escartin, Juan Carlos; Chamorro-Posada, Pedro, E-mail: juagar@yllera.tel.uva.e [Dpto. de TeorIa de la Senal y Comunicaciones e Ingenieria Telematica, Universidad de Valladolid, ETSI de Telecomunicacion, Campus Miguel Delibes, Paseo Belen 15, 47011 Valladolid (Spain)

2010-11-12

Grover's algorithm for quantum search can also be applied to classical energy transfer. The procedure takes a system in which the total energy is equally distributed among N subsystems and transfers most of it to one marked subsystem. We show that in a relativistic setting the efficiency of this procedure can be improved. We will consider the transfer of relativistic kinetic energy in a series of elastic collisions. In this case, the number of steps of the energy transfer procedure approaches 1 as the initial velocities of the objects become closer to the speed of light. This is a consequence of introducing nonlinearities in the procedure. However, the maximum attainable transfer will depend on the particular combination of speed and number of objects. In the procedure, we will use N elements, as in the classical non-relativistic case, instead of the log{sub 2}(N) states of the quantum algorithm.

Blockage of ultrafast and directional diffusion of Li atoms on phosphorene with intrinsic defects.

Science.gov (United States)

Zhang, Ruiqi; Wu, Xiaojun; Yang, Jinlong

2016-02-21

The diffusion of Li in electrode materials is a key factor for the charging/discharging rate capacity of a Li-ion battery (LIB). Recently, two-dimensional phosphorene has been proposed as a very promising electrode material due to its ultrafast and directional lithium diffusion, as well as large energy capacity. Herein, on the basis of density functional theory, we report that intrinsic point defects, including vacancy and stone-wales defects, will block the directional ultrafast diffusion of lithium in phosphorene. On the defect-free phosphorene, diffusion of Li along the zig-zag lattice direction is 1.6 billion times faster than along the armchair lattice direction, and 260 times faster than that in graphite. After introducing intrinsic vacancy and stone-wales defect, the diffusion energy barrier of Li along the zig-zag lattice direction increases sharply to the range of 0.17-0.49 eV, which blocks the ultrafast migration of lithium along the zig-zag lattice direction. Moreover, the open circuit voltage increases with the emergence of defects, which is not suitable for anode materials. In addition, the formation energies of the defects in phosphorene are considerably lower than those in graphene and silicene sheet; therefore, it is highly important to generate defect-free phosphorene for LIB applications.

Impact of local order and stoichiometry on the ultrafast magnetization dynamics of Heusler compounds

International Nuclear Information System (INIS)

Steil, Daniel; Schmitt, Oliver; Fetzer, Roman; Aeschlimann, Martin; Cinchetti, Mirko; Kubota, Takahide; Naganuma, Hiroshi; Oogane, Mikihiko; Ando, Yasuo; Rodan, Steven; Blum, Christian G F; Wurmehl, Sabine; Balke, Benjamin

2015-01-01

Nowadays, a wealth of information on ultrafast magnetization dynamics of thin ferromagnetic films exists in the literature. Information is, however, scarce on bulk single crystals, which may be especially important for the case of multi-sublattice systems. In Heusler compounds, representing prominent examples for such multi-sublattice systems, off-stoichiometry and degree of order can significantly change the magnetic properties of thin films, while bulk single crystals may be generally produced with a much more well-defined stoichiometry and a higher degree of ordering. A careful characterization of the local structure of thin films versus bulk single crystals combined with ultrafast demagnetization studies can, thus, help to understand the impact of stoichiometry and order on ultrafast spin dynamics.Here, we present a comparative study of the structural ordering and magnetization dynamics for thin films and bulk single crystals of the family of Heusler alloys with composition Co 2 Fe 1 − x Mn x Si. The local ordering is studied by 59 Co nuclear magnetic resonance (NMR) spectroscopy, while the time-resolved magneto-optical Kerr effect gives access to the ultrafast magnetization dynamics. In the NMR studies we find significant differences between bulk single crystals and thin films, both regarding local ordering and stoichiometry. The ultrafast magnetization dynamics, on the other hand, turns out to be mostly unaffected by the observed structural differences, especially on the time scale of some hundreds of femtoseconds. These results confirm hole-mediated spin-flip processes as the main mechanism for ultrafast demagnetization and the robustness of this demagnetization channel against defect states in the minority band gap as well as against the energetic position of the band gap with respect to the Fermi energy. The very small differences observed in the magnetization dynamics on the picosecond time-scale, on the other hand, can be explained by considering the

Cooperative photo-induced effects: from photo-magnetism under continuous irradiation to ultra-fast phenomena - study through optical spectroscopy and X-ray diffraction

International Nuclear Information System (INIS)

Glijer, D.

2006-12-01

The control with ultra-short laser pulses of the collective and concerted transformation of molecules driving a macroscopic state switching on an ultra-fast time scale in solid state opens new prospects in materials science. The goal is to realize at the material level what happens at the molecular level in femto-chemistry. These processes are highly cooperative and highly non-linear, leading to self-amplification and self-organization within the material, a so-called photo-induced phase transition with a new long range order (structural, magnetic, ferroelectric,...). Two families of molecular compounds have been studied here: first of all, spin transition materials changing from a diamagnetic state over to a paramagnetic state under the effect of temperature or under continuous laser excitation. It concerns photo-active molecular bi-stability prototype materials in solid state, whose switching has been studied during X-ray diffraction, optical reflectivity and magnetism experiments. Then we have studied charge-transfer molecular systems, prototype compounds for ultrafast photo-induced phase transitions: insulator-metal, neutral-ionic....As well as ultrafast optical experiments, time-resolved X ray crystallography is a key technique in order to follow at the atomic level the different steps of the photo-induced transformation and thus to observe the involved mechanisms. We have underlined a process of photo-formation of one-dimensional nano-domains of lattice-relaxed charge-transfer excitations, governing the photo-induced phase transition of the molecular charge-transfer complex TTF-CA by the first time-resolved diffuse scattering measurements. Moreover, a new femtosecond laser-plasma source and a optical pump-probe spectroscopy set-up with a highly sensitive detecting system have been developed in this work. The results presented here will be an illustration of the present scientific challenges existing on the one hand with the development of projects of major

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

International Nuclear Information System (INIS)

Beni, A; Bogani, L; Bussotti, L; Dei, A; Gentili, P L; Righini, R

2005-01-01

The valence tautomerism of low-spin Co III (Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin Co II (Cat-N-BQ) 2 that, secondly, reaches the chemical equilibrium with the reactant species

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

Science.gov (United States)

Beni, A.; Bogani, L.; Bussotti, L.; Dei, A.; Gentili, P. L.; Righini, R.

2005-01-01

The valence tautomerism of low-spin CoIII(Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin CoII(Cat-N-BQ)2 that, secondly, reaches the chemical equilibrium with the reactant species.

Fusion of Ultraviolet-Visible and Infrared Transient Absorption Spectroscopy Data to Model Ultrafast Photoisomerization.

Science.gov (United States)

Debus, Bruno; Orio, Maylis; Rehault, Julien; Burdzinski, Gotard; Ruckebusch, Cyril; Sliwa, Michel

2017-08-03

Ultrafast photoisomerization reactions generally start at a higher excited state with excess of internal vibrational energy and occur via conical intersections. This leads to ultrafast dynamics which are difficult to investigate with a single transient absorption spectroscopy technique, be it in the ultraviolet-visible (UV-vis) or infrared (IR) domain. On one hand, the information available in the UV-vis domain is limited as only slight spectral changes are observed for different isomers. On the other hand, the interpretation of vibrational spectra is strongly hindered by intramolecular relaxation and vibrational cooling. These limitations can be circumvented by fusing UV-vis and IR transient absorption spectroscopy data in a multiset multivariate curve resolution analysis. We apply this approach to describe the spectrodynamics of the ultrafast cis-trans photoisomerization around the C-N double bond observed for aromatic Schiff bases. Twisted intermediate states could be elucidated, and isomerization was shown to occur through a continuous complete rotation. More broadly, data fusion can be used to rationalize a vast range of ultrafast photoisomerization processes of interest in photochemistry.

Ultrafast dynamics of correlated electrons

Energy Technology Data Exchange (ETDEWEB)

Rettig, Laurenz

2012-07-09

This work investigates the ultrafast electron dynamics in correlated, low-dimensional model systems using femtosecond time- and angle-resolved photoemission spectroscopy (trARPES) directly in the time domain. In such materials, the strong electron-electron (e-e) correlations or coupling to other degrees of freedom such as phonons within the complex many-body quantum system lead to new, emergent properties that are characterized by phase transitions into broken-symmetry ground states such as magnetic, superconducting or charge density wave (CDW) phases. The dynamical processes related to order like transient phase changes, collective excitations or the energy relaxation within the system allow deeper insight into the complex physics governing the emergence of the broken-symmetry state. In this work, several model systems for broken-symmetry ground states and for the dynamical charge balance at interfaces have been studied. In the quantum well state (QWS) model system Pb/Si(111), the charge transfer across the Pb/Si interface leads to an ultrafast energetic stabilization of occupied QWSs, which is the result of an increase of the electronic confinement to the metal film. In addition, a coherently excited surface phonon mode is observed. In antiferromagnetic (AFM) Fe pnictide compounds, a strong momentum-dependent asymmetry of electron and hole relaxation rates allows to separate the recovery dynamics of the AFM phase from electron-phonon (e-ph) relaxation. The strong modulation of the chemical potential by coherent phonon modes demonstrates the importance of e-ph coupling in these materials. However, the average e-ph coupling constant is found to be small. The investigation of the excited quasiparticle (QP) relaxation dynamics in the high-T{sub c}4 superconductor Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+δ} reveals a striking momentum and fluence independence of the QP life times. In combination with the momentum-dependent density of excited QPs, this demonstrates the

Ultrafast laser spectroscopy in complex solid state materials

Energy Technology Data Exchange (ETDEWEB)

Li, Tianqi [Iowa State Univ., Ames, IA (United States)

2014-12-01

This thesis summarizes my work on applying the ultrafast laser spectroscopy to the complex solid state materials. It shows that the ultrafast laser pulse can coherently control the material properties in the femtosecond time scale. And the ultrafast laser spectroscopy can be employed as a dynamical method for revealing the fundamental physical problems in the complex material systems.

An estimate of spherical impactor energy transfer for mechanical frequency up-conversion energy harvester

Directory of Open Access Journals (Sweden)

L. R. Corr

2016-08-01

Full Text Available Vibration energy harvesters, which use the impact mechanical frequency up-conversion technique, utilize an impactor, which gains kinetic energy from low frequency ambient environmental vibrations, to excite high frequency systems that efficiently convert mechanical energy to electrical energy. To take full advantage of the impact mechanical frequency up-conversion technique, it is prudent to understand the energy transfer from the low frequency excitations, to the impactor, and finally to the high frequency systems. In this work, the energy transfer from a spherical impactor to a multi degree of freedom spring / mass system, due to Hertzian impact, is investigated to gain insight on how best to design impact mechanical frequency up-conversion energy harvesters. Through this academic work, it is shown that the properties of the contact (or impact area, i.e., radius of curvature and material properties, only play a minor role in energy transfer and that the equivalent mass of the target system (i.e., the spring / mass system dictates the total amount of energy transferred during the impact. The novel approach of utilizing the well-known Hertzian impact methodology to gain an understanding of impact mechanical frequency up-conversion energy harvesters has made it clear that the impactor and the high frequency energy generating systems must be designed together as one system to ensure maximum energy transfer, leading to efficient ambient vibration energy harvesters.

Efficient near-field wireless energy transfer using adiabatic system variations

Energy Technology Data Exchange (ETDEWEB)

Hamam, Rafif E.; Karalis, Aristeidis; Joannopoulos, John D.; Soljacic, Marin

2017-11-28

Disclosed is a method for transferring energy wirelessly including transferring energy wirelessly from a first resonator structure to an intermediate resonator structure, wherein the coupling rate between the first resonator structure and the intermediate resonator structure is .kappa..sub.1B, transferring energy wirelessly from the intermediate resonator structure to a second resonator structure, wherein the coupling rate between the intermediate resonator structure and the second resonator structure is .kappa..sub.B2, and during the wireless energy transfers, adjusting at least one of the coupling rates .kappa..sub.1B and .kappa..sub.B2 to reduce energy accumulation in the intermediate resonator structure and improve wireless energy transfer from the first resonator structure to the second resonator structure through the intermediate resonator structure.

Wireless energy transfer between anisotropic metamaterials shells

Energy Technology Data Exchange (ETDEWEB)

Díaz-Rubio, Ana; Carbonell, Jorge; Sánchez-Dehesa, José, E-mail: jsdehesa@upv.es

2014-06-15

The behavior of strongly coupled Radial Photonic Crystals shells is investigated as a potential alternative to transfer electromagnetic energy wirelessly. These sub-wavelength resonant microstructures, which are based on anisotropic metamaterials, can produce efficient coupling phenomena due to their high quality factor. A configuration of selected constitutive parameters (permittivity and permeability) is analyzed in terms of its resonant characteristics. The coupling to loss ratio between two coupled resonators is calculated as a function of distance, the maximum (in excess of 300) is obtained when the shells are separated by three times their radius. Under practical conditions an 83% of maximum power transfer has been also estimated. -- Highlights: •Anisotropic metamaterial shells exhibit high quality factors and sub-wavelength size. •Exchange of electromagnetic energy between shells with high efficiency is analyzed. •Strong coupling is supported with high wireless transfer efficiency. •End-to-end energy transfer efficiencies higher than 83% can be predicted.

Wireless energy transfer between anisotropic metamaterials shells

International Nuclear Information System (INIS)

Díaz-Rubio, Ana; Carbonell, Jorge; Sánchez-Dehesa, José

2014-01-01

The behavior of strongly coupled Radial Photonic Crystals shells is investigated as a potential alternative to transfer electromagnetic energy wirelessly. These sub-wavelength resonant microstructures, which are based on anisotropic metamaterials, can produce efficient coupling phenomena due to their high quality factor. A configuration of selected constitutive parameters (permittivity and permeability) is analyzed in terms of its resonant characteristics. The coupling to loss ratio between two coupled resonators is calculated as a function of distance, the maximum (in excess of 300) is obtained when the shells are separated by three times their radius. Under practical conditions an 83% of maximum power transfer has been also estimated. -- Highlights: •Anisotropic metamaterial shells exhibit high quality factors and sub-wavelength size. •Exchange of electromagnetic energy between shells with high efficiency is analyzed. •Strong coupling is supported with high wireless transfer efficiency. •End-to-end energy transfer efficiencies higher than 83% can be predicted

Four-Dimensional Ultrafast Electron Microscopy: Insights into an Emerging Technique

KAUST Repository

Adhikari, Aniruddha

2016-12-15

Four-dimensional ultrafast electron microscopy (4D-UEM) is a novel analytical technique that aims to fulfill the long-held dream of researchers to investigate materials at extremely short spatial and temporal resolutions by integrating the excellent spatial resolution of electron microscopes with the temporal resolution of ultrafast femtosecond laser-based spectroscopy. The ingenious use of pulsed photoelectrons to probe surfaces and volumes of materials enables time-resolved snapshots of the dynamics to be captured in a way hitherto impossible by other conventional techniques. The flexibility of 4D-UEM lies in the fact that it can be used in both the scanning (S-UEM) and transmission (UEM) modes depending upon the type of electron microscope involved. While UEM can be employed to monitor elementary structural changes and phase transitions in samples using real-space mapping, diffraction, electron energy-loss spectroscopy, and tomography, S-UEM is well suited to map ultrafast dynamical events on materials surfaces in space and time. This review provides an overview of the unique features that distinguish these techniques and also illustrates the applications of both S-UEM and UEM to a multitude of problems relevant to materials science and chemistry.

Spectral Gap Energy Transfer in Atmospheric Boundary Layer

Science.gov (United States)

Bhushan, S.; Walters, K.; Barros, A. P.; Nogueira, M.

2012-12-01

Experimental measurements of atmospheric turbulence energy spectra show E(k) ~ k-3 slopes at synoptic scales (~ 600 km - 2000 km) and k-5/3 slopes at the mesoscales (theory, it is expected that a strong backward energy cascade would develop at the synoptic scale, and that circulation would grow infinitely. To limit this backward transfer, energy arrest at macroscales must be introduced. The most commonly used turbulence models developed to mimic the above energy transfer include the energy backscatter model for 2D turbulence in the horizontal plane via Large Eddy Simulation (LES) models, dissipative URANS models in the vertical plane, and Ekman friction for the energy arrest. One of the controversial issues surrounding the atmospheric turbulence spectra is the explanation of the generation of the 2D and 3D spectra and transition between them, for energy injection at the synoptic scales. Lilly (1989) proposed that the existence of 2D and 3D spectra can only be explained by the presence of an additional energy injection in the meso-scale region. A second issue is related to the observations of dual peak spectra with small variance in meso-scale, suggesting that the energy transfer occurs across a spectral gap (Van Der Hoven, 1957). Several studies have confirmed the spectral gap for the meso-scale circulations, and have suggested that they are enhanced by smaller scale vertical convection rather than by the synoptic scales. Further, the widely accepted energy arrest mechanism by boundary layer friction is closely related to the spectral gap transfer. This study proposes an energy transfer mechanism for atmospheric turbulence with synoptic scale injection, wherein the generation of 2D and 3D spectra is explained using spectral gap energy transfer. The existence of the spectral gap energy transfer is validated by performing LES for the interaction of large scale circulation with a wall, and studying the evolution of the energy spectra both near to and far from the wall

Influence of donor-donor transport on excitation energy transfer

Energy Technology Data Exchange (ETDEWEB)

Pandey, K K; Joshi, H C; Pant, T C [Kumaun University, Nainital (India). Department of Physics

1989-01-01

Energy migration and transfer from acriflavine to rhodamine B and malachite green in poly (methylmethacrylate) have been investigated using the decay function analysis. It is found that the influence of energy migration in energy transfer can be described quite convincingly by making use of the theories of Loring, Andersen and Fayer (LAF) and Huber. At high acceptor concentration direct donor-acceptor transfer occurs through Forster mechanism. (author). 17 refs., 5 figs.

Ultrafast time-resolved spectroscopy of xanthophylls at low temperature.

Science.gov (United States)

Cong, Hong; Niedzwiedzki, Dariusz M; Gibson, George N; Frank, Harry A

2008-03-20

Many of the spectroscopic features and photophysical properties of xanthophylls and their role in energy transfer to chlorophyll can be accounted for on the basis of a three-state model. The characteristically strong visible absorption of xanthophylls is associated with a transition from the ground state S0 (1(1)Ag-) to the S2 (1(1)Bu+) excited state. The lowest lying singlet state denoted S1 (2(1)Ag-), is a state into which absorption from the ground state is symmetry forbidden. Ultrafast optical spectroscopic studies and quantum computations have suggested the presence of additional excited singlet states in the vicinity of S1 (2(1)Ag-) and S2 (1(1)Bu+). One of these is denoted S* and has been suggested in previous work to be associated with a twisted molecular conformation of the molecule in the S1 (2(1)Ag-) state. In this work, we present the results of a spectroscopic investigation of three major xanthophylls from higher plants: violaxanthin, lutein, and zeaxanthin. These molecules have systematically increasing extents of pi-electron conjugation from nine to eleven conjugated carbon-carbon double bonds. All-trans isomers of the molecules were purified by high-performance liquid chromatography (HPLC) and studied by steady-state and ultrafast time-resolved optical spectroscopy at 77 K. Analysis of the data using global fitting techniques has revealed the inherent spectral properties and ultrafast dynamics of the excited singlet states of each of the molecules. Five different global fitting models were tested, and it was found that the data are best explained using a kinetic model whereby photoexcitation results in the promotion of the molecule into the S2 (1(1)Bu+) state that subsequently undergoes decay to a vibrationally hot S1 (1(1)Ag-) state and with the exception of violaxanthin also to the S* state. The vibrationally hot S1 (1(1)Ag-) state then cools to a vibrationally relaxed S1 (2(1)Ag-) state in less than a picosecond. It was also found that a portion

Energy transfer in reactive and non-reactive H2 + OH collisions

International Nuclear Information System (INIS)

Rashed, O.; Brown, N.J.

1985-04-01

We have used the methods of quasi-classical dynamics to compute energy transfer properties of non-reactive and reactive H 2 + OH collisions. Energy transfer has been investigated as function of translational temperature, reagent rotational energy, and reagent vibrational energy. The energy transfer mechanism is complex with ten types of energy transfer possible, and evidence was found for all types. There is much more exchange between the translational degree of freedom and the H 2 vibrational degree of freedom than there is between translation and OH vibration. Translational energy is transferred to the rotational degrees of freedom of each molecule. There is a greater propensity for the transfer of translation to OH rotation than H 2 rotation. In reactive collisions, increases in reagent translational temperature predominantly appear as vibrational energy in the water molecule. Energy transfer in non-reactive and reactive collisions does not depend strongly on the initial angular momentum in either molecule. In non-reactive collisions, vibrational energy is transferred to translation, to the rotational degree of freedom of the same molecule, and to the rotational and vibrational degrees of freedom of the other molecule. In reactive collisions, the major effect of increasing the vibrational energy in reagent molecules is that, on the average, the vibrational energy of the reagents appears as product vibrational energy. 18 refs., 16 figs., 6 tabs

New Aspects of Photocurrent Generation at Graphene pn Junctions Revealed by Ultrafast Optical Measurements

Science.gov (United States)

Aivazian, Grant; Sun, Dong; Jones, Aaron; Ross, Jason; Yao, Wang; Cobden, David; Xu, Xiaodong

2012-02-01

The remarkable electrical and optical properties of graphene make it a promising material for new optoelectronic applications. However, one important, but so far unexplored, property is the role of hot carriers in charge and energy transport at graphene interfaces. Here we investigate the photocurrent (PC) dynamics at a tunable graphene pn junction using ultrafast scanning PC microscopy. Pump-probe measurements show a temperature dependent relaxation time of photogenerated carriers that increases from 1.5ps at 290K to 4ps at 20K; while the amplitude of the PC is independent of the lattice temperature. These observations imply that it is hot carriers, not phonons, which dominate ultrafast energy transport. Gate dependent measurements show many interesting features such as pump induced saturation, enhancement, and sign reversal of probe generated PC. These observations reveal that the underlying PC mechanism is a combination of the thermoelectric and built-in electric field effects. Our results enhance the understanding of non-equilibrium electron dynamics, electron-electron interactions, and electron-phonon interactions in graphene. They also determine fundamental limits on ultrafast device operation speeds (˜500 GHz) for graphene-based photodetectors.

Energy-donor phosphorescence quenching study of triplet–triplet energy transfer between UV absorbers

International Nuclear Information System (INIS)

Kikuchi, Azusa; Nakabai, Yuya; Oguchi-Fujiyama, Nozomi; Miyazawa, Kazuyuki; Yagi, Mikio

2015-01-01

The intermolecular triplet–triplet energy transfer from a photounstable UV-A absorber, 4-tert-butyl-4′-methoxydibenzoylmethane (BMDBM), to UV-B absorbers, 2-ethylhexyl 4-methoxycinnamate (octyl methoxycinnamate, OMC), octocrylene (OCR) and dioctyl 4-methoxybenzylidenemalonate (DOMBM) has been observed using a 355 nm laser excitation in rigid solutions at 77 K. The decay curves of the energy-donor phosphorescence in the presence of the UV-B absorbers deviate from the exponential decay at the initial stage of the decay. The Stern–Volmer formulation is not valid in rigid solutions because molecular diffusion is impossible. The experimental results indicate that the rate constant of triplet–triplet energy transfer from BMDBM to the UV-B absorbers, k T–T , decreases in the following order: k T–T (BMDBM–DOMBM)>k T–T (BMDBM–OMC)≥k T–T (BMDBM–OCR). The presence of DOMBM enhances the photostability of the widely used combination of UV-A and UV-B absorbers, BMDBM and OCR. The effects of the triplet–triplet energy transfer on the photostability of BMDBM are discussed. - Highlights: • The intermolecular triplet–triplet energy transfer between UV absorbers was observed. • The phosphorescence decay deviates from exponential at the initial stage of decay. • The effects of triplet–triplet energy transfer on the photostability are discussed

The impact of electrostatic interactions on ultrafast charge transfer at Ag 29 nanoclusters–fullerene and CdTe quantum dots–fullerene interfaces

KAUST Repository

Ahmed, Ghada H.

2015-11-09

A profound understanding of charge transfer (CT) at semiconductor quantum dots (QDs) and nanoclusters (NCs) interfaces is extremely important to optimize the energy conversion efficiency in QDs and NCs-based solar cell devices. Here, we report on the ground- and excited-state interactions at the interface of two different bimolecular non-covalent donor-acceptor (D-A) systems using steady-state and femtosecond transient absorption (fs-TA) spectroscopy with broadband capabilities. We systematically investigate the electrostatic interactions between the positively charged fullerene derivative C60-(N,N dimethylpyrrolidinium iodide) (CF) employed as an efficient molecular acceptor and two different donor molecules: Ag29 nanoclusters (NCs) and CdTe quantum dots (QDs). For comparison purposes, we also monitor the interaction of each donor molecule with the neutral fullerene derivative C60-(malonic acid)n, which has minimal electrostatic interactions. Our steady-state and time-resolved data demonstrate that both QDs and NCs have strong interfacial electrostatic interactions and dramatic fluorescence quenching when the CF derivative is present. In other words, our results reveal that only CF can be in close molecular proximity with the QDs and NCs, allowing ultrafast photoinduced CT to occur. It turned out that the intermolecular distances, electronic coupling and subsequently CT from the excited QDs or NCs to fullerene derivatives can be controlled by the interfacial electrostatic interactions. Our findings highlight some of the key variable components for optimizing CT at QDs and NCs interfaces, which can also be applied to other D-A systems that rely on interfacial CT. © The Royal Society of Chemistry 2016.

A simplified approach for the coupling of excitation energy transfer

Energy Technology Data Exchange (ETDEWEB)

Shi Bo [Hefei National Laboratory for Physical Science at Microscale, University of Science and Technology of China, Hefei 230026 (China); Department of Chemical Physics, University of Science and Technology of China, Hefei 230026 (China); Gao Fang, E-mail: gaofang@iim.ac.cn [Institute of Intelligent Machines, Chinese Academy of Sciences, Hefei 230031 (China); State Key Laboratory of Robotics, Shenyang Institute of Automation, Chinese Academy of Sciences, Shenyang 110016 (China); Liang Wanzhen [Hefei National Laboratory for Physical Science at Microscale, University of Science and Technology of China, Hefei 230026 (China); Department of Chemical Physics, University of Science and Technology of China, Hefei 230026 (China)

2012-02-06

Highlights: Black-Right-Pointing-Pointer We propose a simple method to calculate the coupling of singlet-to-singlet and triplet-to-triplet energy transfer. Black-Right-Pointing-Pointer Coulomb term are the major contribution to the coupling of singlet-to-singlet energy transfer. Black-Right-Pointing-Pointer Effect from the intermolecular charge-transfer states dorminates in triplet-to-triplet energy transfer. Black-Right-Pointing-Pointer This method can be expanded by including correlated wavefunctions. - Abstract: A simplified approach for computing the electronic coupling of nonradiative excitation-energy transfer is proposed by following Scholes et al.'s construction on the initial and final states [G.D. Scholes, R.D. Harcourt, K.P. Ghiggino, J. Chem. Phys. 102 (1995) 9574]. The simplification is realized through defining a set of orthogonalized localized MOs, which include the polarization effect of the charge densities. The method allows calculating the coupling of both the singlet-to-singlet and triplet-to-triplet energy transfer. Numerical tests are performed for a few of dimers with different intermolecular orientations, and the results demonstrate that Coulomb term are the major contribution to the coupling of singlet-to-singlet energy transfer whereas in the case of triplet-to-triplet energy transfer, the dominant effect is arisen from the intermolecular charge-transfer states. The present application is on the Hartree-Fock level. However, the correlated wavefunctions which are normally expanded in terms of the determinant wavefunctions can be employed in the similar way.

Risk transfer via energy savings insurance; TOPICAL

International Nuclear Information System (INIS)

Mills, Evan

2001-01-01

Among the key barriers to investment in energy efficiency improvements are uncertainties about attaining projected energy savings and apprehension about potential disputes over these savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building commissioning), financial risk transfer techniques are less developed in the energy management arena than in other more mature segments of the economy. Energy Savings Insurance (ESI) - formal insurance of predicted energy savings - is one method of transferring financial risks away from the facility owner or energy services contractor. ESI offers a number of significant advantages over other forms of financial risk transfer, e.g. savings guarantees or performance bonds. ESI providers manage risk via pre-construction design review as well as post-construction commissioning and measurement and verification of savings. We found that the two mos t common criticisms of ESI - excessive pricing and onerous exclusions - are not born out in practice. In fact, if properly applied, ESI can potentially reduce the net cost of energy savings projects by reducing the interest rates charged by lenders, and by increasing the level of savings through quality control. Debt service can also be ensured by matching loan payments to projected energy savings while designing the insurance mechanism so that payments are made by the insurer in the event of a savings shortfall. We estimate the U.S. ESI market potential of$875 million/year in premium income. From an energy-policy perspective, ESI offers a number of potential benefits: ESI transfers performance risk from the balance sheet of the entity implementing the energy savings project, thereby freeing up capital otherwise needed to ''self-insure'' the savings. ESI reduces barriers to market entry of smaller energy services firms who do not have sufficiently strong balance sheets to self

Excited-state intramolecular hydrogen transfer (ESIHT) of 1,8-Dihydroxy-9,10-anthraquinone (DHAQ) characterized by ultrafast electronic and vibrational spectroscopy and computational modeling

KAUST Repository

Mohammed, Omar F.

2014-05-01

We combine ultrafast electronic and vibrational spectroscopy and computational modeling to investigate the photoinduced excited-state intramolecular hydrogen-transfer dynamics in 1,8-dihydroxy-9,10-anthraquinone (DHAQ) in tetrachloroethene, acetonitrile, dimethyl sulfoxide, and methanol. We analyze the electronic excited states of DHAQ with various possible hydrogen-bonding schemes and provide a general description of the electronic excited-state dynamics based on a systematic analysis of femtosecond UV/vis and UV/IR pump-probe spectroscopic data. Upon photoabsorption at 400 nm, the S 2 electronic excited state is initially populated, followed by a rapid equilibration within 150 fs through population transfer to the S 1 state where DHAQ exhibits ESIHT dynamics. In this equilibration process, the excited-state population is distributed between the 9,10-quinone (S2) and 1,10-quinone (S1) states while undergoing vibrational energy redistribution, vibrational cooling, and solvation dynamics on the 0.1-50 ps time scale. Transient UV/vis pump-probe data in methanol also suggest additional relaxation dynamics on the subnanosecond time scale, which we tentatively ascribe to hydrogen bond dynamics of DHAQ with the protic solvent, affecting the equilibrium population dynamics within the S2 and S1 electronic excited states. Ultimately, the two excited singlet states decay with a solvent-dependent time constant ranging from 139 to 210 ps. The concomitant electronic ground-state recovery is, however, only partial because a large fraction of the population relaxes to the first triplet state. From the similarity of the time scales involved, we conjecture that the solvent plays a crucial role in breaking the intramolecular hydrogen bond of DHAQ during the S2/S1 relaxation to either the ground or triplet state. © 2014 American Chemical Society.

Mid-range adiabatic wireless energy transfer via a mediator coil

International Nuclear Information System (INIS)

Rangelov, A.A.; Vitanov, N.V.

2012-01-01

A technique for efficient mid-range wireless energy transfer between two coils via a mediator coil is proposed. By varying the coil frequencies, three resonances are created: emitter–mediator (EM), mediator–receiver (MR) and emitter–receiver (ER). If the frequency sweeps are adiabatic and such that the EM resonance precedes the MR resonance, the energy flows sequentially along the chain emitter–mediator–receiver. If the MR resonance precedes the EM resonance, then the energy flows directly from the emitter to the receiver via the ER resonance; then the losses from the mediator are suppressed. This technique is robust against noise, resonant constraints and external interferences. - Highlights: ► Efficient and robust mid-range wireless energy transfer via a mediator coil. ► The adiabatic energy transfer is analogous to adiabatic passage in quantum optics. ► Wireless energy transfer is insensitive to any resonant constraints. ► Wireless energy transfer is insensitive to noise in the neighborhood of the coils.

Bimodal Exciplex Formation in Bimolecular Photoinduced Electron Transfer Revealed by Ultrafast Time-Resolved Infrared Absorption.

Science.gov (United States)

Koch, Marius; Licari, Giuseppe; Vauthey, Eric

2015-09-03

The dynamics of a moderately exergonic photoinduced charge separation has been investigated by ultrafast time-resolved infrared absorption with the dimethylanthracene/phthalonitrile donor/acceptor pair in solvents covering a broad range of polarity. A distinct spectral signature of an exciplex could be identified in the -C≡N stretching region. On the basis of quantum chemistry calculations, the 4-5 times larger width of this band compared to those of the ions and of the locally excited donor bands is explained by a dynamic distribution of exciplex geometry with different mutual orientations and distances of the constituents and, thus, with varying charge-transfer character. Although spectrally similar, two types of exciplexes could be distinguished by their dynamics: short-lived, "tight", exciplexes generated upon static quenching and longer-lived, "loose", exciplexes formed upon dynamic quenching in parallel with ion pairs. Tight exciplexes were observed in all solvents, except in the least polar diethyl ether where quenching is slower than diffusion. The product distribution of the dynamic quenching depends strongly on the solvent polarity: whereas no significant loose exciplex population could be detected in acetonitrile, both exciplex and ion pair are generated in less polar solvents, with the relative population of exciplex increasing with decreasing solvent polarity. These results are compared with those reported previously with donor/acceptor pairs in different driving force regimes to obtain a comprehensive picture of the role of the exciplexes in bimolecular photoinduced charge separation.

Characterization of photo-induced valence tautomerism in a cobalt-dioxolene complex by ultrafast spectroscopy

Energy Technology Data Exchange (ETDEWEB)

Beni, A [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy); Bogani, L [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy); Bussotti, L [LENS, Universita di Firenze, Via Nello Carrara 1, 50019 Sesto Fiorentino, Florence (Italy); Dei, A [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy); Gentili, P L [LENS, Universita di Firenze, Via Nello Carrara 1, 50019 Sesto Fiorentino, Florence (Italy); Righini, R [Dipartimento di Chimica, Universita di Firenze, via della Lastruccia 3, 50019 Sesto Fiorentino, Florence (Italy)

2005-01-01

The valence tautomerism of low-spin Co{sup III}(Cat-N-BQ)(Cat-N-SQ) was investigated by means of UV-vis pump-probe transient absorption spectroscopy in chloroform. By exciting the CT transition of the complex at 480 nm, an intramolecular electron transfer process is selectively triggered. The photo-induced charge transfer is pursued by a cascade of two main molecular events characterized by the ultrafast transient absorption spectroscopy: the first gives rise to the metastable high-spin Co{sup II}(Cat-N-BQ){sub 2} that, secondly, reaches the chemical equilibrium with the reactant species.

Mode-to-mode energy transfers in convective patterns

Indian Academy of Sciences (India)

Abstract. We investigate the energy transfer between various Fourier modes in a low- dimensional model for thermal convection. We have used the formalism of mode-to-mode energy transfer rate in our calculation. The evolution equations derived using this scheme is the same as those derived using the hydrodynamical ...

Ultrafast Electric Field Pulse Control of Giant Temperature Change in Ferroelectrics

Science.gov (United States)

Qi, Y.; Liu, S.; Lindenberg, A. M.; Rappe, A. M.

2018-01-01

There is a surge of interest in developing environmentally friendly solid-state-based cooling technology. Here, we point out that a fast cooling rate (≈1011 K /s ) can be achieved by driving solid crystals to a high-temperature phase with a properly designed electric field pulse. Specifically, we predict that an ultrafast electric field pulse can cause a giant temperature decrease up to 32 K in PbTiO3 occurring on few picosecond time scales. We explain the underlying physics of this giant electric field pulse-induced temperature change with the concept of internal energy redistribution: the electric field does work on a ferroelectric crystal and redistributes its internal energy, and the way the kinetic energy is redistributed determines the temperature change and strongly depends on the electric field temporal profile. This concept is supported by our all-atom molecular dynamics simulations of PbTiO3 and BaTiO3 . Moreover, this internal energy redistribution concept can also be applied to understand electrocaloric effect. We further propose new strategies for inducing giant cooling effect with ultrafast electric field pulse. This Letter offers a general framework to understand electric-field-induced temperature change and highlights the opportunities of electric field engineering for controlled design of fast and efficient cooling technology.

Protonation-induced ultrafast torsional dynamics in 9-anthrylbenzimidazole: a pH activated molecular rotor.

Science.gov (United States)

Nandi, Amitabha; Kushwaha, Archana; Das, Dipanwita; Ghosh, Rajib

2018-03-07

We report the photophysical properties and excited state dynamics of 9-anthrylbenzimidazole (ANBI) which exhibits protonation-induced molecular rotor properties. In contrast to the highly emissive behavior of neutral ANBI, protonation of the benzimidazole group of ANBI induces efficient nonradiative deactivation by ultrafast torsional motion around the bond connecting the anthracene and benzimidazole units, as revealed by ultrafast transient absorption and fluorescence spectroscopy. Contrary to viscosity-independent fluorescence of neutral dyes, protonated ANBI is shown to display linear variation of emission yield and lifetime with solvent viscosity. The protonation-induced molecular rotor properties in the studied system are shown to be driven by enhanced charge transfer and are corroborated by quantum chemical calculations. Potential application as a microviscosity sensor of acidic regions in a heterogeneous environment by these proton-activated molecular rotor properties of ANBI is discussed.

Quantum electrodynamics of resonant energy transfer in condensed matter

International Nuclear Information System (INIS)

Juzeliunas, G.; Andrews, D.L.

1994-01-01

A microscopic many-body QED theory for dipole-dipole resonance energy transfer has been developed from first principles. A distinctive feature of the theory is full incorporation of the dielectric effects of the supporting medium. The approach employs the concept of bath polaritons mediating the energy transfer. The transfer rate is derived in terms of the Green's operator corresponding to the polariton matrix Hamiltonian. In contrast to the more common lossless polariton models, the present theory accommodates an arbitrary number of energy levels for each molecule of the medium. This includes, a case of special interest, where the excitation energy spectrum of the bath molecules is sufficiently dense that it can be treated as a quasicontinuum in the energy region in question, as in the condensed phase normally results from homogeneous and inhomogeneous line broadening. In such a situation, the photon ''dressed'' by the medium polarization (the polariton) acquires a finite lifetime, the role of the dissipative subsystem being played by bath molecules. It is this which leads to the appearance of the exponential decay factor in the microscopically derived pair transfer rates. Accordingly, the problem associated with potentially infinite total ensemble rates, due to the divergent R -2 contribution, is solved from first principles. In addition, the medium modifies the distance dependence of the energy transfer function A(R) and also produces extra modifications due to screening contributions and local field effects. The formalism addresses cases where the surrounding medium is either absorbing or lossless over the range of energies transferred. In the latter case the exponential factor does not appear and the dielectric medium effect in the near zone reduces to that which is familiar from the theory of radiationless (Foerster) energy transfer

Damage of DNA by Low Energy Electrons (< 3 eV)

International Nuclear Information System (INIS)

Bald, Ilko; Illenberger, Eugen; Kopyra, Janina

2012-01-01

Recent experiments on low energy electron attachment to DNA and its components in the condensed phase and in the gas phase are reviewed and analysed. From different condensed phase experiments the sensitivity of DNA towards low energy electrons is well documented and strand breaks in DNA are observed at subexcitation energies (< 3 eV) and also in ultrafast electron transfer experiments involving electrons in presolvated states. Gas phase experiments indicate that all building blocks of DNA (the nucleobases, the sugar and the phosphate moiety) undergo resonant dissociative electron attachment (DEA) in the subexcitation regime which may ultimately lead to strand breaks. From very recent gas phase experiments on an entire nucleotide it can be concluded that most strand breaks result from direct electron attachment to the DNA backbone, but also initial electron capture by the nucleobase following electron transfer to the backbone contributes.

Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode.

Science.gov (United States)

Bücker, K; Picher, M; Crégut, O; LaGrange, T; Reed, B W; Park, S T; Masiel, D J; Banhart, F

2016-12-01

High temporal resolution transmission electron microscopy techniques have shown significant progress in recent years. Using photoelectron pulses induced by ultrashort laser pulses on the cathode, these methods can probe ultrafast materials processes and have revealed numerous dynamic phenomena at the nanoscale. Most recently, the technique has been implemented in standard thermionic electron microscopes that provide a flexible platform for studying material's dynamics over a wide range of spatial and temporal scales. In this study, the electron pulses in such an ultrafast transmission electron microscope are characterized in detail. The microscope is based on a thermionic gun with a Wehnelt electrode and is operated in a stroboscopic photoelectron mode. It is shown that the Wehnelt bias has a decisive influence on the temporal and energy spread of the picosecond electron pulses. Depending on the shape of the cathode and the cathode-Wehnelt distance, different emission patterns with different pulse parameters are obtained. The energy spread of the pulses is determined by space charge and Boersch effects, given by the number of electrons in a pulse. However, filtering effects due to the chromatic aberrations of the Wehnelt electrode allow the extraction of pulses with narrow energy spreads. The temporal spread is governed by electron trajectories of different length and in different electrostatic potentials. High temporal resolution is obtained by excluding shank emission from the cathode and aberration-induced halos in the emission pattern. By varying the cathode-Wehnelt gap, the Wehnelt bias, and the number of photoelectrons in a pulse, tradeoffs between energy and temporal resolution as well as beam intensity can be made as needed for experiments. Based on the characterization of the electron pulses, the optimal conditions for the operation of ultrafast TEMs with thermionic gun assembly are elaborated. Copyright © 2016 Elsevier B.V. All rights reserved.

Generation of mega-electron-volt electron beams by an ultrafast intense laser pulse

International Nuclear Information System (INIS)

Wang Xiaofang; Saleh, Ned; Krishnan, Mohan; Wang Haiwen; Backus, Sterling; Murnane, Margaret; Kapteyn, Henry; Umstadter, Donald; Wang Quandong; Shen Baifei

2003-01-01

Mega-electron-volt (MeV) electron emission from the interaction of an ultrafast (τ∼29 fs), intense (>10 18 W/cm 2 ) laser pulse with underdense plasmas has been studied. A beam of MeV electrons with a divergence angle as small as 1 deg. is observed in the forward direction, which is correlated with relativistic filamentation of the laser pulse in plasmas. A novel net-energy-gain mechanism is proposed for electron acceleration resulting from the relativistic filamentation and beam breakup. These results suggest an approach for generating a beam of femtosecond, MeV electrons at a kilohertz repetition rate with a compact ultrafast intense laser system

Risk transfer via energy savings insurance

OpenAIRE

Mills, Evan

2001-01-01

Among the key barriers to investment in energy efficiency improvements are uncertainties about attaining projected energy savings and apprehension about potential disputes over these savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building commissioning), financial risk transfer techniques are less developed in the energy management arena than in other more mature segments of t...

Intramolecular photoinduced electron-transfer in azobenzene-perylene diimide

International Nuclear Information System (INIS)

Feng Wen-Ke; Wang Shu-Feng; Gong Qi-Huang; Feng Yi-Yu; Feng Wei; Yi Wen-Hui

2010-01-01

This paper studies the intramolecular photoinduced electron-transfer (PET) of covalent bonded azobenzene-perylene diimide (AZO-PDI) in solvents by using steady-state and time-resolved fluorescence spectroscopy together with ultrafast transient absorption spectroscopic techniques. Fast fluorescence quenching is observed when AZO-PDI is excited at characteristic wavelengths of AZO and perylene moieties. Reductive electron-transfer with transfer rate faster than 10 11 s −1 is found. This PET process is also consolidated by femtosecond transient absorption spectra

Ultrafast palladium diffusion in germanium

KAUST Repository

Tahini, Hassan Ali

2015-01-01

The slow transport of dopants through crystal lattices has hindered the development of novel devices. Typically atoms are contained within deep potential energy wells which necessitates multiple attempts to hop between minimum energy positions. This is because the bonds that constrain atoms are strongest at the minimum positions. As they hop between sites the bonds must be broken, only to re-form as the atoms slide into adjacent minima. Here we demonstrate that the Pd atoms introduced into the Ge lattice behave differently. They retain bonds as the atoms shift across so that at the energy maximum between sites Pd still exhibits strong bonding characteristics. This reduces the energy maximum to almost nothing (a migration energy of only 0.03 eV) and means that the transport of Pd through the Ge lattice is ultrafast. We scrutinize the bonding characteristics at the atomic level using quantum mechanical simulation tools and demonstrate why Pd behaves so differently to other metals we investigated (i.e. Li, Cu, Ag, Pt and Au). Consequently, this fundamental understanding can be extended to systems where extremely rapid diffusion is desired, such as radiation sensors, batteries and solid oxide fuel cells.

How Does Thymine DNA Survive Ultrafast Dimerization Damage?

Directory of Open Access Journals (Sweden)

Hongjuan Wang

2016-12-01

Full Text Available The photodimerization reaction between the two adjacent thymine bases within a single strand has been the subject of numerous studies due to its potential to induce DNA mutagenesis and possible tumorigenesis in human skin cells. It is well established that the cycloaddition photoreaction takes place on a picosecond time scale along barrierless or low barrier singlet/triplet pathways. However, the observed dimerization quantum yield in different thymine multimer is considerable lower than might be expected. A reasonable explanation is required to understand why thymine in DNA is able to survive ultrafast dimerization damage. In this work, accurate quantum calculations based on the combined CASPT2//CASSCF/AMBER method were conducted to map the excited state relaxation pathways of the thymine monomer in aqueous solution and of the thymine oligomer in DNA. A monomer-like decay pathway, induced by the twisting of the methyl group, is found to provide a bypass channel to ensure the photostability of thymine in single-stranded oligomers. This fast relaxation path is regulated by the conical intersection between the bright SCT(1ππ* state with the intra-base charge transfer character and the ground state to remove the excess excitation energy, thereby achieving the ground-state recovery with high efficiency.

Non-equilibrium lattice dynamics of one-dimensional In chains on Si(111 upon ultrafast optical excitation

Directory of Open Access Journals (Sweden)

T. Frigge

2018-03-01

Full Text Available The photoinduced structural dynamics of the atomic wire system on the Si(111-In surface has been studied by ultrafast electron diffraction in reflection geometry. Upon intense fs-laser excitation, this system can be driven in around 1 ps from the insulating (8×2 reconstructed low temperature phase to a metastable metallic (4×1 reconstructed high temperature phase. Subsequent to the structural transition, the surface heats up on a 6 times slower timescale as determined from a transient Debye-Waller analysis of the diffraction spots. From a comparison with the structural response of the high temperature (4×1 phase, we conclude that electron-phonon coupling is responsible for the slow energy transfer from the excited electron system to the lattice. The significant difference in timescales is evidence that the photoinduced structural transition is non-thermally driven.

Ultrafast time-resolved spectroscopy of the light-harvesting complex 2 (LH2) from the photosynthetic bacterium Thermochromatium tepidum.

Science.gov (United States)

Niedzwiedzki, Dariusz M; Fuciman, Marcel; Kobayashi, Masayuki; Frank, Harry A; Blankenship, Robert E

2011-10-01

The light-harvesting complex 2 from the thermophilic purple bacterium Thermochromatium tepidum was purified and studied by steady-state absorption and fluorescence, sub-nanosecond-time-resolved fluorescence and femtosecond time-resolved transient absorption spectroscopy. The measurements were performed at room temperature and at 10 K. The combination of both ultrafast and steady-state optical spectroscopy methods at ambient and cryogenic temperatures allowed the detailed study of carotenoid (Car)-to-bacteriochlorophyll (BChl) as well BChl-to-BChl excitation energy transfer in the complex. The studies show that the dominant Cars rhodopin (N=11) and spirilloxanthin (N=13) do not play a significant role as supportive energy donors for BChl a. This is related with their photophysical properties regulated by long π-electron conjugation. On the other hand, such properties favor some of the Cars, particularly spirilloxanthin (N=13) to play the role of the direct quencher of the excited singlet state of BChl. © Springer Science+Business Media B.V. 2011

Theory of coherent resonance energy transfer

International Nuclear Information System (INIS)

Jang, Seogjoo; Cheng, Y.-C.; Reichman, David R.; Eaves, Joel D.

2008-01-01

A theory of coherent resonance energy transfer is developed combining the polaron transformation and a time-local quantum master equation formulation, which is valid for arbitrary spectral densities including common modes. The theory contains inhomogeneous terms accounting for nonequilibrium initial preparation effects and elucidates how quantum coherence and nonequilibrium effects manifest themselves in the coherent energy transfer dynamics beyond the weak resonance coupling limit of the Foerster and Dexter (FD) theory. Numerical tests show that quantum coherence can cause significant changes in steady state donor/acceptor populations from those predicted by the FD theory and illustrate delicate cooperation of nonequilibrium and quantum coherence effects on the transient population dynamics.

A novel optical tool for controlling and probing ultrafast surface dynamics

International Nuclear Information System (INIS)

Yang, Yudong

2017-12-01

Ultrashort pulse laser sources have been greatly developed over the past few decades. The available pulse duration has been reduced to the single-cycle pulse regime. The discovery of high harmonic generation has freed us from the limitation of the laser wavelength. Moreover, the demonstration of isolated attosecond pulse generation has indicated the advent of the attosecond science era. Attosecond pulses undoubtedly allow one to study ultrafast dynamics with unprecedented time resolution. However, physical systems with genuine attosecond time scale dynamics are rather challenging to find. Ultrafast surface charge transfer, which is an important process in photochemistry and electrochemistry, is a good candidate experimental system exhibiting attosecond electronic dynamics. Specifically, the ultrafast surface charge transfer on the c(4 x 2)S/Ru(0001) surface was previously studied and the charge transfer time inferred to be 320 as using core-hole clock spectroscopy at a synchrotron facility. In order to measure this benchmark attosecond electronic dynamics with real time-resolving methods, pump pulses centered at 160 eV and probe pulses centered at 40 eV are required. To this end, a dedicated attosecond experimental beamline including an ultrashort laser pulse source and an attosecond pulse generation and characterization setup has been designed and is being developed. The author of this thesis was responsible for the construction of the attosecond experimental beamline which will be used ultrafast surface charge transfer studies. In this thesis, a completely functional attosecond extreme ultraviolet (XUV) beamline, which includes a few-cycle laser pulse source, an attosecond pulse generation and characterization setup, is described. A commercial Ti:sapphire-based chirped-pulse amplification (CPA) laser system is the overall source of the beamline. The laser system is actively carrier-envelope phase (CEP) stabilized and the output pulse duration is ∝35 fs. The

A novel optical tool for controlling and probing ultrafast surface dynamics

Energy Technology Data Exchange (ETDEWEB)

Yang, Yudong

2017-12-15

Ultrashort pulse laser sources have been greatly developed over the past few decades. The available pulse duration has been reduced to the single-cycle pulse regime. The discovery of high harmonic generation has freed us from the limitation of the laser wavelength. Moreover, the demonstration of isolated attosecond pulse generation has indicated the advent of the attosecond science era. Attosecond pulses undoubtedly allow one to study ultrafast dynamics with unprecedented time resolution. However, physical systems with genuine attosecond time scale dynamics are rather challenging to find. Ultrafast surface charge transfer, which is an important process in photochemistry and electrochemistry, is a good candidate experimental system exhibiting attosecond electronic dynamics. Specifically, the ultrafast surface charge transfer on the c(4 x 2)S/Ru(0001) surface was previously studied and the charge transfer time inferred to be 320 as using core-hole clock spectroscopy at a synchrotron facility. In order to measure this benchmark attosecond electronic dynamics with real time-resolving methods, pump pulses centered at 160 eV and probe pulses centered at 40 eV are required. To this end, a dedicated attosecond experimental beamline including an ultrashort laser pulse source and an attosecond pulse generation and characterization setup has been designed and is being developed. The author of this thesis was responsible for the construction of the attosecond experimental beamline which will be used ultrafast surface charge transfer studies. In this thesis, a completely functional attosecond extreme ultraviolet (XUV) beamline, which includes a few-cycle laser pulse source, an attosecond pulse generation and characterization setup, is described. A commercial Ti:sapphire-based chirped-pulse amplification (CPA) laser system is the overall source of the beamline. The laser system is actively carrier-envelope phase (CEP) stabilized and the output pulse duration is ∝35 fs. The

First-principles assessment of potential ultrafast laser-induced structural transition in Ni

Energy Technology Data Exchange (ETDEWEB)

Bévillon, E.; Colombier, J.P., E-mail: jean.philippe.colombier@univ-st-etienne.fr; Stoian, R.

2016-06-30

Highlights: • First-principles theory calculations in nonequilibrium conditions. • Electronic temperatures fully and consistently taken into account. • Evaluation of an ultrafast laser-induced solid-to-solid transition in Ni. • Relative energies, phonon spectra and energy path are evaluated. • Discussion on the generation of non-thermal forces in metals. - Abstract: The possibility to trigger ultrafast solid-to-solid transitions in transition metals under femtosecond laser irradiation is investigated by means of first-principles calculations. Electronic heating can drastically modify screening, charge distribution and atomic binding features, potentially determining new structural relaxation paths in the solid phase, before thermodynamic solid-to-liquid transformations set in. Consequently, we evaluate here the effect of electronic excitation on structural stability and conditions for structural transitions. Ni is chosen as a case study for the probability of a solid transition, and the stability of its FCC phase is compared to the non-standard HCP structure while accounting for the heating of the electronic subsystem. From a phonon spectra analysis, we show that the thermodynamic stability order reverses at an electronic temperature of around 10{sup 4} K. Both structures exhibit a dynamic stability, indicating they present a metastability depending on the heating. However, the general hardening of phonon modes with the increase of the electronic temperature points out that no transformation will occur, as confirmed by the study of a typical FCC to HCP diffusionless transformation path, showing an increasing energy barrier. Finally, based on electronic density of states interpretation, the tendency of different metal categories to undergo or not an ultrafast laser-induced structural transition is discussed.

Developing a structure-function model for the cryptophyte phycoerythrin 545 using ultrahigh resolution crystallography and ultrafast laser spectroscopy.

Science.gov (United States)

Doust, Alexander B; Marai, Christopher N J; Harrop, Stephen J; Wilk, Krystyna E; Curmi, Paul M G; Scholes, Gregory D

2004-11-12

Cryptophyte algae differ from cyanobacteria and red algae in the architecture of their photosynthetic light harvesting systems, even though all three are evolutionarily related. Central to cryptophyte light harvesting is the soluble antenna protein phycoerythrin 545 (PE545). The ultrahigh resolution crystal structure of PE545, isolated from a unicellular cryptophyte Rhodomonas CS24, is reported at both 1.1A and 0.97A resolution, revealing details of the conformation and environments of the chromophores. Absorption, emission and polarized steady state spectroscopy (298K, 77K), as well as ultrafast (20fs time resolution) measurements of population dynamics are reported. Coupled with complementary quantum chemical calculations of electronic transitions of the bilins, these enable assignment of spectral absorption characteristics to each chromophore in the structure. Spectral differences between the tetrapyrrole pigments due to chemical differences between bilins, as well as their binding and interaction with the local protein environment are described. Based on these assignments, and considering customized optical properties such as strong coupling, a model for light harvesting by PE545 is developed which explains the fast, directional harvesting of excitation energy. The excitation energy is funnelled from four peripheral pigments (beta158,beta82) into a central chromophore dimer (beta50/beta61) in approximately 1ps. Those chromophores, in turn, transfer the excitation energy to the red absorbing molecules located at the periphery of the complex in approximately 4ps. A final resonance energy transfer step sensitizes just one of the alpha19 bilins on a time scale of 22ps. Furthermore, it is concluded that binding of PE545 to the thylakoid membrane is not essential for efficient energy transfer to the integral membrane chlorophyll a-containing complexes associated with PS-II.

Photoinduced Electron Transfer in the Strong Coupling Regime: Waveguide-Plasmon Polaritons.

Science.gov (United States)

Zeng, Peng; Cadusch, Jasper; Chakraborty, Debadi; Smith, Trevor A; Roberts, Ann; Sader, John E; Davis, Timothy J; Gómez, Daniel E

2016-04-13

Reversible exchange of photons between a material and an optical cavity can lead to the formation of hybrid light-matter states where material properties such as the work function [ Hutchison et al. Adv. Mater. 2013 , 25 , 2481 - 2485 ], chemical reactivity [ Hutchison et al. Angew. Chem., Int. Ed. 2012 , 51 , 1592 - 1596 ], ultrafast energy relaxation [ Salomon et al. Angew. Chem., Int. Ed. 2009 , 48 , 8748 - 8751 ; Gomez et al. J. Phys. Chem. B 2013 , 117 , 4340 - 4346 ], and electrical conductivity [ Orgiu et al. Nat. Mater. 2015 , 14 , 1123 - 1129 ] of matter differ significantly to those of the same material in the absence of strong interactions with the electromagnetic fields. Here we show that strong light-matter coupling between confined photons on a semiconductor waveguide and localized plasmon resonances on metal nanowires modifies the efficiency of the photoinduced charge-transfer rate of plasmonic derived (hot) electrons into accepting states in the semiconductor material. Ultrafast spectroscopy measurements reveal a strong correlation between the amplitude of the transient signals, attributed to electrons residing in the semiconductor and the hybridization of waveguide and plasmon excitations.

Precision machining of pig intestine using ultrafast laser pulses

Science.gov (United States)

Beck, Rainer J.; Góra, Wojciech S.; Carter, Richard M.; Gunadi, Sonny; Jayne, David; Hand, Duncan P.; Shephard, Jonathan D.

2015-07-01

Endoluminal surgery for the treatment of early stage colorectal cancer is typically based on electrocautery tools which imply restrictions on precision and the risk of harm through collateral thermal damage to the healthy tissue. As a potential alternative to mitigate these drawbacks we present laser machining of pig intestine by means of picosecond laser pulses. The high intensities of an ultrafast laser enable nonlinear absorption processes and a predominantly nonthermal ablation regime. Laser ablation results of square cavities with comparable thickness to early stage colorectal cancers are presented for a wavelength of 1030 nm using an industrial picosecond laser. The corresponding histology sections exhibit only minimal collateral damage to the surrounding tissue. The depth of the ablation can be controlled precisely by means of the pulse energy. Overall, the application of ultrafast lasers to ablate pig intestine enables significantly improved precision and reduced thermal damage to the surrounding tissue compared to conventional techniques.

Ultrafast electronic relaxation of excited state vitamin B12 in the gas phase

International Nuclear Information System (INIS)

Shafizadeh, Niloufar; Poisson, Lionel; Soep, Benoit

2008-01-01

The time evolution of electronically excited vitamin B 12 (cyanocobalamin) has been observed for the first time in the gas phase. It reveals an ultrafast decay to a state corresponding to metal excitation. This decay is interpreted as resulting from a ring to metal electron transfer. This opens the observation of the excited state of other complex biomimetic systems in the gas phase, the key to the characterisation of their complex evolution through excited electronic states

Pair transfer processes probed at deep sub barrier energies

International Nuclear Information System (INIS)

Corradi, L.; Mason, P.; Fioretto, E.; Michelagnoli, C.; Stefanini, A.M.; Valiente-Dobon, J.J.; Szinler, S.; Jelavic-Malenica, D.; Soic, N.; Pollarolo, G.; Farnea, E.; Montagnoli, G.; Montanari, D.; Scarlassara, F.; Ur, C.A.; Gadea, A.; Haas, F.; Marginean, N.

2011-01-01

Multinucleon transfer cross sections in the system 40 Ca+ 96 Zr have been measured at bombarding energies ranging from the Coulomb barrier to ∼ 25% below. Target-like (lighter) recoils in inverse kinematics have been completely identified in A,Z and Q-value with the large solid angle magnetic spectrometer PRISMA. The experimental slopes of the neutron transfer probabilities at large internuclear separation are consistent with the values derived from the binding energies. A phenomenological interpretation of the transfer probabilities indicates the presence of enhanced values for the even number of neutron transfers. (authors)

Laser-driven ultrafast antiproton beam

Science.gov (United States)

Li, Shun; Pei, Zhikun; Shen, Baifei; Xu, Jiancai; Zhang, Lingang; Zhang, Xiaomei; Xu, Tongjun; Yu, Yong; Bu, Zhigang

2018-02-01

Antiproton beam generation is investigated based on the ultra-intense femtosecond laser pulse by using two-dimensional particle-in-cell and Geant4 simulations. A high-flux proton beam with an energy of tens of GeV is generated in sequential radiation pressure and bubble regime and then shoots into a high-Z target for producing antiprotons. Both yield and energy of the antiproton beam increase almost linearly with the laser intensity. The generated antiproton beam has a short pulse duration of about 5 ps and its flux reaches 2 × 10 20 s - 1 at the laser intensity of 2.14 × 10 23 W / cm 2 . Compared to conventional methods, this new method based on the ultra-intense laser pulse is able to provide a compact, tunable, and ultrafast antiproton source, which is potentially useful for quark-gluon plasma study, all-optical antihydrogen generation, and so on.

Ultrafast intramolecular relaxation dynamics of Mg- and Zn-bacteriochlorophyll a

Energy Technology Data Exchange (ETDEWEB)

Kosumi, Daisuke [Osaka City University Advanced Research Institute for Natural Science and Technology, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Nakagawa, Katsunori; Sakai, Shunsuke [Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); Nagaoka, Yuya; Maruta, Satoshi; Sugisaki, Mitsuru [CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); Dewa, Takehisa [Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); PRESTO/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Nango, Mamoru [The Osaka City University Advanced Research Institute for Natural Science and Technology, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); Hashimoto, Hideki [The Osaka City University Advanced Research Institute for Natural Science and Technology, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan); CREST/JST, 4-1-8 Honcho, Kawaguchi, Saitama 332-0012 (Japan); Department of Physics, Graduate School of Science, Osaka City University, 3-3-138 Sugimoto, Sumiyoshi-ku, Osaka 558-8585 (Japan)

2013-07-21

Ultrafast excited-state dynamics of the photosynthetic pigment (Mg-)bacteriochlorophyll a and its Zn-substituted form were investigated by steady-state absorption/fluorescence and femtosecond pump-probe spectroscopic measurements. The obtained steady-state absorption and fluorescence spectra of bacteriochlorophyll a in solution showed that the central metal compound significantly affects the energy of the Q{sub x} state, but has almost no effect on the Q{sub y} state. Photo-induced absorption spectra were recorded upon excitation of Mg- and Zn-bacteriochlorophyll a into either their Q{sub x} or Q{sub y} state. By comparing the kinetic traces of transient absorption, ground-state beaching, and stimulated emission after excitation to the Q{sub x} or Q{sub y} state, we showed that the Q{sub x} state was substantially incorporated in the ultrafast excited-state dynamics of bacteriochlorophyll a. Based on these observations, the lifetime of the Q{sub x} state was determined to be 50 and 70 fs for Mg- and Zn-bacteriochlorophyll a, respectively, indicating that the lifetime was influenced by the central metal atom due to the change of the energy gap between the Q{sub x} and Q{sub y} states.

Ultrafast Carbon Dioxide Sorption Kinetics Using Lithium Silicate Nanowires.

Science.gov (United States)

Nambo, Apolo; He, Juan; Nguyen, Tu Quang; Atla, Veerendra; Druffel, Thad; Sunkara, Mahendra

2017-06-14

In this paper, the Li 4 SiO 4 nanowires (NWs) were shown to be promising for CO 2 capture with ultrafast kinetics. Specifically, the nanowire powders exhibited an uptake of 0.35 g g -1 of CO 2 at an ultrafast adsorption rate of 0.22 g g -1 min -1 at 650-700 °C. Lithium silicate (Li 4 SiO 4 ) nanowires and nanopowders were synthesized using a "solvo-plasma" technique involving plasma oxidation of silicon precursors mixed with lithium hydroxide. The kinetic parameter values (k) extracted from sorption kinetics obtained using NW powders are 1 order of magnitude higher than those previously reported for the Li 4 SiO 4 -CO 2 reaction system. The time scales for CO 2 sorption using nanowires are approximately 3 min and two orders magnitude faster compared to those obtained using lithium silicate powders with spherical morphologies and aggregates. Furthermore, Li 4 SiO 4 nanowire powders showed reversibility through sorption-desorption cycles indicating their suitability for CO 2 capture applications. All of the morphologies of Li 4 SiO 4 powders exhibited a double exponential behavior in the adsorption kinetics indicating two distinct time constants for kinetic and the mass transfer limited regimes.

Power law scaling for rotational energy transfer

International Nuclear Information System (INIS)

Pritchard, D.E.; Smith, N.; Driver, R.D.; Brunner, T.A.

1979-01-01

We have applied a new scaling law to several sets of rotational energy transfer cross sections. The new law asserts that the square of the T-matrix depends on the amount of energy transferred as a power law. Two different kinds of angular momentum statistics are assumed, one corresponding to m/sub j/ being conserved and the other corresponding to m/sub j/ being completely randomized. Numerical fits are presented which demonstrate that the data follow the power law better than the widely used exponential gap law

Coherent excitation-energy transfer and quantum entanglement in a dimer

International Nuclear Information System (INIS)

Liao Jieqiao; Sun, C. P.; Huang Jinfeng; Kuang Leman

2010-01-01

We study coherent energy transfer of a single excitation and quantum entanglement in a dimer, which consists of a donor and an acceptor modeled by two two-level systems. Between the donor and the acceptor, there exists a dipole-dipole interaction, which provides the physical mechanism for coherent energy transfer and entanglement generation. The donor and the acceptor couple to two independent heat baths with diagonal couplings that do not dissipate the energy of the noncoupling dimer. Special attention is paid to the effect on single-excitation energy transfer and entanglement generation of the energy detuning between the donor and the acceptor and the temperatures of the two heat baths. It is found that, the probability for single-excitation energy transfer largely depends on the energy detuning in the low temperature limit. Concretely, the positive and negative energy detunings can increase and decrease the probability at steady state, respectively. In the high temperature limit, however, the effect of the energy detuning on the probability is negligibly small. We also find that the probability is negligibly dependent on the bath temperature difference of the two heat baths. In addition, it is found that quantum entanglement can be generated in the process of coherent energy transfer. As the bath temperature increases, the generated steady-state entanglement decreases. For a given bath temperature, the steady-state entanglement decreases with the increase of the absolute value of the energy detuning.

Progress in ultrafast laser processing and future prospects

Science.gov (United States)

Sugioka, Koji

2017-03-01

The unique characteristics of ultrafast lasers have rapidly revolutionized materials processing after their first demonstration in 1987. The ultrashort pulse width of the laser suppresses heat diffusion to the surroundings of the processed region, which minimizes the formation of a heat-affected zone and thereby enables ultrahigh precision micro- and nanofabrication of various materials. In addition, the extremely high peak intensity can induce nonlinear multiphoton absorption, which extends the diversity of materials that can be processed to transparent materials such as glass. Nonlinear multiphoton absorption enables three-dimensional (3D) micro- and nanofabrication by irradiation with tightly focused femtosecond laser pulses inside transparent materials. Thus, ultrafast lasers are currently widely used for both fundamental research and practical applications. This review presents progress in ultrafast laser processing, including micromachining, surface micro- and nanostructuring, nanoablation, and 3D and volume processing. Advanced technologies that promise to enhance the performance of ultrafast laser processing, such as hybrid additive and subtractive processing, and shaped beam processing are discussed. Commercial and industrial applications of ultrafast laser processing are also introduced. Finally, future prospects of the technology are given with a summary.

Optical Nonlinearities and Ultrafast Carrier Dynamics in Semiconductor Quantum Dots

Energy Technology Data Exchange (ETDEWEB)

Klimov, V.; McBranch, D.; Schwarz, C.

1998-08-10

Low-dimensional semiconductors have attracted great interest due to the potential for tailoring their linear and nonlinear optical properties over a wide-range. Semiconductor nanocrystals (NC's) represent a class of quasi-zero-dimensional objects or quantum dots. Due to quantum cordhement and a large surface-to-volume ratio, the linear and nonlinear optical properties, and the carrier dynamics in NC's are significantly different horn those in bulk materials. napping at surface states can lead to a fast depopulation of quantized states, accompanied by charge separation and generation of local fields which significantly modifies the nonlinear optical response in NC's. 3D carrier confinement also has a drastic effect on the energy relaxation dynamics. In strongly confined NC's, the energy-level spacing can greatly exceed typical phonon energies. This has been expected to significantly inhibit phonon-related mechanisms for energy losses, an effect referred to as a phonon bottleneck. It has been suggested recently that the phonon bottleneck in 3D-confined systems can be removed due to enhanced role of Auger-type interactions. In this paper we report femtosecond (fs) studies of ultrafast optical nonlinearities, and energy relaxation and trap ping dynamics in three types of quantum-dot systems: semiconductor NC/glass composites made by high temperature precipitation, ion-implanted NC's, and colloidal NC'S. Comparison of ultrafast data for different samples allows us to separate effects being intrinsic to quantum dots from those related to lattice imperfections and interface properties.

Design and synthesis of bipyridine platinum(II) bisalkynyl fullerene donor-chromophore-acceptor triads with ultrafast charge separation.

Science.gov (United States)

Lee, Sai-Ho; Chan, Chris Tsz-Leung; Wong, Keith Man-Chung; Lam, Wai Han; Kwok, Wai-Ming; Yam, Vivian Wing-Wah

2014-07-16

Donor-chromophore-acceptor triads, (PTZ)2-Pt(bpy)-C60 and ((t)BuPTZ)2-Pt(bpy)-C60, along with their model compound, (Ph)2-Pt(bpy)-C60, have been synthesized and characterized; their photophysical and electrochemical properties have been studied, and the origin of the absorption and emission properties has been supported by computational studies. The photoinduced electron transfer reactions have been investigated using the femtosecond and nanosecond transient absorption spectroscopy. In dichloromethane, (Ph)2-Pt(bpy)-C60 shows ultrafast triplet-triplet energy transfer from the (3)MLCT/LLCT excited state within 4 ps to give the (3)C60* state, while in (PTZ)2-Pt(bpy)-C60 and ((t)BuPTZ)2-Pt(bpy)-C60, charge-separated state forms within 400 fs from the (3)MLCT/LLCT excited state with efficiency of over 0.90, and the total efficiency with the contribution of (3)C60* is estimated to be 0.99. Although the forward electron transfer reactions are very rapid, the charge-separated state recombines to the singlet ground state at a time of hundreds of nanoseconds because of the difference in spin multiplicity between the charge-separated state and the ground state.

Energy transfer in porous anodic alumina/rhodamine 110 nanocomposites

Energy Technology Data Exchange (ETDEWEB)

Elhouichet, H., E-mail: habib.elhouichet@fst.rnu.tn [Laboratoire de Physico-Chimie des Materiaux Mineraux et leurs Applications, Centre National de Recherches en Sciences des Materiaux, B.P. 95, Hammam-Lif 2050 (Tunisia); Departement de Physique, Faculte des Sciences de Tunis, University of Tunis Elmanar 2092 Tunis (Tunisia); Harima, N.; Koyama, H. [Hyogo University of Teacher Education, Kato, Hyogo 673-1494 (Japan); Gaponenko, N.V. [Belarusian State University of Informatics and Radioelectronics, P. Browki St. 6, 220013 Minsk (Belarus)

2012-09-15

We have used porous anodic alumina (PAA) films as templates for embedding rhodamine 110 (Rh110) molecules and examined their photoluminescence (PL) properties in detail. The analysis of the polarization memory (PM) of PL strongly suggests that there is a significant energy transfer from PAA to Rh110 molecules. The effect of annealing the PAA layer on the PL properties of the nanocomposite has been studied. The results show that the energy transfer becomes more efficient in annealed PAA. - Highlights: Black-Right-Pointing-Pointer Porous anodic alumina-rhodamine 110 nanocomposites are elaborated. Black-Right-Pointing-Pointer Efficient energy transfer from the host to Rh110 molecules is evidenced from measurements of photoluminescence and degree of polarization memory spectra. Black-Right-Pointing-Pointer Thermal annealing of porous anodic alumina can improve the process of excitation transfer.

Energy transfer in a mechanically trapped exciplex.

Science.gov (United States)

Klosterman, Jeremy K; Iwamura, Munetaka; Tahara, Tahei; Fujita, Makoto

2009-07-15

Host-guest complexes involving M(6)L(4) coordination cages can display unusual photoreactivity, and enclathration of the very large fluorophore bisanthracene resulted in an emissive, mechanically trapped intramolecular exciplex. Mechanically linked intramolecular exciplexes are important for understanding the dependence of energy transfer on donor-acceptor distance, orientation, and electronic coupling but are relatively unexplored. Steady-state and picosecond time-resolved fluorescence measurements have revealed that selective excitation of the encapsulated guest fluorophore results in efficient energy transfer from the excited guest to an emissive host-guest exciplex state.

Nuclear response functions at large energy and momentum transfer

International Nuclear Information System (INIS)

Bertozzi, W.; Moniz, E.J.; Lourie, R.W.

1991-01-01

Quasifree nucleon processes are expected to dominate the nuclear electromagnetic response function for large energy and momentum transfers, i.e., for energy transfers large compared with nuclear single particle energies and momentum transfers large compared with typical nuclear momenta. Despite the evident success of the quasifree picture in providing the basic frame work for discussing and understanding the large energy, large momentum nuclear response, the limits of this picture have also become quite clear. In this article a selected set of inclusive and coincidence data are presented in order to define the limits of the quasifree picture more quantitatively. Specific dynamical mechanisms thought to be important in going beyond the quasifree picture are discussed as well. 75 refs, 37 figs

Computational study of energy transfer in two-dimensional J-aggregates

International Nuclear Information System (INIS)

Gallos, Lazaros K.; Argyrakis, Panos; Lobanov, A.; Vitukhnovsky, A.

2004-01-01

We perform a computational analysis of the intra- and interband energy transfer in two-dimensional J-aggregates. Each aggregate is represented as a two-dimensional array (LB-film or self-assembled film) of two kinds of cyanine dyes. We consider the J-aggregate whose J-band is located at a shorter wavelength to be a donor and an aggregate or a small impurity with longer wavelength to be an acceptor. Light absorption in the blue wing of the donor aggregate gives rise to the population of its excitonic states. The depopulation of these states is possible by (a) radiative transfer to the ground state (b) intraband energy transfer, and (c) interband energy transfer to the acceptor. We study the dependence of energy transfer on properties such as the energy gap, the diagonal disorder, and the exciton-phonon interaction strength. Experimentally observable parameters, such as the position and form of luminescence spectrum, and results of the kinetic spectroscopy measurements strongly depend upon the density of states in excitonic bands, rates of energy exchange between states and oscillator strengths for luminescent transitions originating from these states

Energy technology transfer to developing countries

International Nuclear Information System (INIS)

Goldemberg, J.

1991-01-01

This paper gives some examples of how technology transfer can successfully be given to third world countries to allow them to benefit in their quest for economic growth and better standards of living through reduced energy consumption and environmental pollution. It also suggests methods by which obstacles such as high investment costs, lack of information, market demand, etc., can be overcome in order to motivate technological transfer by industrialized countries

Definition and determination of the triplet-triplet energy transfer reaction coordinate.

Science.gov (United States)

Zapata, Felipe; Marazzi, Marco; Castaño, Obis; Acuña, A Ulises; Frutos, Luis Manuel

2014-01-21

A definition of the triplet-triplet energy transfer reaction coordinate within the very weak electronic coupling limit is proposed, and a novel theoretical formalism is developed for its quantitative determination in terms of internal coordinates The present formalism permits (i) the separation of donor and acceptor contributions to the reaction coordinate, (ii) the identification of the intrinsic role of donor and acceptor in the triplet energy transfer process, and (iii) the quantification of the effect of every internal coordinate on the transfer process. This formalism is general and can be applied to classical as well as to nonvertical triplet energy transfer processes. The utility of the novel formalism is demonstrated here by its application to the paradigm of nonvertical triplet-triplet energy transfer involving cis-stilbene as acceptor molecule. In this way the effect of each internal molecular coordinate in promoting the transfer rate, from triplet donors in the low and high-energy limit, could be analyzed in detail.

Perspective: Ultrafast magnetism and THz spintronics

Energy Technology Data Exchange (ETDEWEB)

Walowski, Jakob; Münzenberg, Markus [Institut für Physik, Ernst-Moritz-Arndt-Universität Greifswald, 17489 Greifswald (Germany)

2016-10-14

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

Perspective: Ultrafast magnetism and THz spintronics

International Nuclear Information System (INIS)

Walowski, Jakob; Münzenberg, Markus

2016-01-01

This year the discovery of femtosecond demagnetization by laser pulses is 20 years old. For the first time, this milestone work by Bigot and coworkers gave insight directly into the time scales of microscopic interactions that connect the spin and electron system. While intense discussions in the field were fueled by the complexity of the processes in the past, it now became evident that it is a puzzle of many different parts. Rather than providing an overview that has been presented in previous reviews on ultrafast processes in ferromagnets, this perspective will show that with our current depth of knowledge the first applications are developed: THz spintronics and all-optical spin manipulation are becoming more and more feasible. The aim of this perspective is to point out where we can connect the different puzzle pieces of understanding gathered over 20 years to develop novel applications. Based on many observations in a large number of experiments. Differences in the theoretical models arise from the localized and delocalized nature of ferromagnetism. Transport effects are intrinsically non-local in spintronic devices and at interfaces. We review the need for multiscale modeling to address the processes starting from electronic excitation of the spin system on the picometer length scale and sub-femtosecond time scale, to spin wave generation, and towards the modeling of ultrafast phase transitions that altogether determine the response time of the ferromagnetic system. Today, our current understanding gives rise to the first usage of ultrafast spin physics for ultrafast magnetism control: THz spintronic devices. This makes the field of ultrafast spin-dynamics an emerging topic open for many researchers right now.

Intramolecular singlet-singlet energy transfer in antenna-substituted azoalkanes.

Science.gov (United States)

Pischel, Uwe; Huang, Fang; Nau, Werner M

2004-03-01

Two novel azoalkane bichromophores and related model compounds have been synthesised and photophysically characterised. Dimethylphenylsiloxy (DPSO) or dimethylnaphthylsiloxy (DNSO) serve as aromatic donor groups (antenna) and the azoalkane 2,3-diazabicyclo[2.2.2]oct-2-ene (DBO) as the acceptor. The UV spectral window of DBO (250-300 nm) allows selective excitation of the donor. Intramolecular singlet-singlet energy transfer to DBO is highly efficient and proceeds with quantum yields of 0.76 with DPSO and 0.99 with DNSO. The photophysical and spectral properties of the bichromophoric systems suggest that energy transfer occurs through diffusional approach of the donor and acceptor within a van der Waals contact at which the exchange mechanism is presumed to dominate. Furthermore, akin to the behaviour of electron-transfer systems in the Marcus inverted region, a rate of energy transfer 2.5 times slower was observed for the system with the more favourable energetics, i.e. singlet-singlet energy transfer from DPSO proceeded slower than from DNSO, although the process is more exergonic for DPSO (-142 kJ mol(-1) for DPSO versus-67 kJ mol(-1) for DNSO).

Energy transfer from a superconducting magnet to an inductive load

International Nuclear Information System (INIS)

Onishi, Toshitada; Miura, Akinori.

1977-01-01

Experiments on energy transfer between two superconducting magnets have been carried out using an inductive energy transfer system similar to the flying capacitor system developed at the Karlsruhe Institute. In the present system the capacitor is grounded and diodes are used instead of thyristors, and a fraction of stored energy is transferred to the capacitor only when the relay connected in parallel to the magnet is switched off. The capacitor is expected to have no constraint in size, while in the flying capacitor system the capacitor is required to exceed a threshold size. Consequently it is possible to shorten the transfer time to some extent in comparison with the one in the flying capacitor system. Transfer experiments have been carried out using a storage magnet with inductance of 1.2H and a load of 0.41H. The capacitance is 200μF. It is possible to transfer 80.1% of the stored energy of 221 J into the load in less than about 0.35 seconds. (auth.)

Energy transfer in diatom/diatom molecular collisions

International Nuclear Information System (INIS)

Sohlberg, K.W.

1992-01-01

In a collision of two molecules, the translational energy of the collision may be redistributed into internal energy of rotation, vibration, or electron motion, in one or both of the colliding partners. In addition, internal energy in one or more of these modes may be open-quotes quenchedclose quotes into translation, leading to a superelastic collision. Such energy transfer may take place by a number of mechanisms. This energy transfer is of fundamental importance in understanding chemical reaction dynamics. Nearly all chemical reactions take place through a bimolecular collision process (or multiple bimolecular collisions) and the quantum state specificity of the reaction can have a major role in determining the kinetics of the reaction, In particular, the author has investigated vibrational energy transfer in collisions between two diatomic molecules. In addition to serving as models for all molecular collision process, gas phase collisions of these species are ubiquitous in atmospheric phenomena which are of critical importance in answering the current questions about the human induced degradation of the earth's atmospheric. Classical trajectory methods have been used to explore the excitation of vibrations in gas-phase collisions of the nitrogen molecular ion with its parent molecule. The near symmetry of the reactants is shown to result in a high probability that the two molecules are excited by an equal amount of energy. This provides a possible explanation of the molecular beam measurements which show that the total number of vibrational energy quanta excited in the collision is, with a high probability that the two molecules are excited by an equal amount of energy. This provides a possible explanation of the molecular beam measurements which show that the total number of vibrational energy quanta excited in the collision is, with a high probability, even

Energy transfers in dynamos with small magnetic Prandtl numbers

KAUST Repository

Kumar, Rohit

2015-06-25

We perform numerical simulation of dynamo with magnetic Prandtl number Pm = 0.2 on 10243 grid, and compute the energy fluxes and the shell-to-shell energy transfers. These computations indicate that the magnetic energy growth takes place mainly due to the energy transfers from large-scale velocity field to large-scale magnetic field and that the magnetic energy flux is forward. The steady-state magnetic energy is much smaller than the kinetic energy, rather than equipartition; this is because the magnetic Reynolds number is near the dynamo transition regime. We also contrast our results with those for dynamo with Pm = 20 and decaying dynamo. © 2015 Taylor & Francis.

FPS-vidicon television camras for ultrafast-scan data acquisition

International Nuclear Information System (INIS)

Noel, B.W.; Yates, G.J.

1980-06-01

Two ultrafast-scan ( 500 TV lines per picture height with a corresponding dynamic range (to light input) of more than 100. The cameras use the unique properties of FPS vidicons and specially designed electronics to achieve their performance levels and versatility. The advantages and disadvantages of FPS vidicons and of antimony trisulfide and silicon target materials in such applications are discussed in detail. All of the electronics circuits are discussed. The sweep generator designs are treated at length because they are the key to the cameras' versatility. Emphasis is placed on remotely controllable analog and digital sweep generators. The latter is a complete CAMAC-compatible subsystem containing a 16-function master arithmetic logic unit. Pulsed and cw methods of obtaining transfer characteristics are described and compared. The effects of generation rates, tube types, and target types on the resolution, determined from contrast-transfer-function curves, are discussed. Several applications are described, including neutron TV pinhole, TREAT, and barium-release experiments

Organic solar cells: understanding the role of Förster resonance energy transfer.

Science.gov (United States)

Feron, Krishna; Belcher, Warwick J; Fell, Christopher J; Dastoor, Paul C

2012-12-12

Organic solar cells have the potential to become a low-cost sustainable energy source. Understanding the photoconversion mechanism is key to the design of efficient organic solar cells. In this review, we discuss the processes involved in the photo-electron conversion mechanism, which may be subdivided into exciton harvesting, exciton transport, exciton dissociation, charge transport and extraction stages. In particular, we focus on the role of energy transfer as described by F¨orster resonance energy transfer (FRET) theory in the photoconversion mechanism. FRET plays a major role in exciton transport, harvesting and dissociation. The spectral absorption range of organic solar cells may be extended using sensitizers that efficiently transfer absorbed energy to the photoactive materials. The limitations of F¨orster theory to accurately calculate energy transfer rates are discussed. Energy transfer is the first step of an efficient two-step exciton dissociation process and may also be used to preferentially transport excitons to the heterointerface, where efficient exciton dissociation may occur. However, FRET also competes with charge transfer at the heterointerface turning it in a potential loss mechanism. An energy cascade comprising both energy transfer and charge transfer may aid in separating charges and is briefly discussed. Considering the extent to which the photo-electron conversion efficiency is governed by energy transfer, optimisation of this process offers the prospect of improved organic photovoltaic performance and thus aids in realising the potential of organic solar cells.

Organic Solar Cells: Understanding the Role of Förster Resonance Energy Transfer

Directory of Open Access Journals (Sweden)

Paul C. Dastoor

2012-12-01

Full Text Available Organic solar cells have the potential to become a low-cost sustainable energy source. Understanding the photoconversion mechanism is key to the design of efficient organic solar cells. In this review, we discuss the processes involved in the photo-electron conversion mechanism, which may be subdivided into exciton harvesting, exciton transport, exciton dissociation, charge transport and extraction stages. In particular, we focus on the role of energy transfer as described by F¨orster resonance energy transfer (FRET theory in the photoconversion mechanism. FRET plays a major role in exciton transport, harvesting and dissociation. The spectral absorption range of organic solar cells may be extended using sensitizers that efficiently transfer absorbed energy to the photoactive materials. The limitations of F¨orster theory to accurately calculate energy transfer rates are discussed. Energy transfer is the first step of an efficient two-step exciton dissociation process and may also be used to preferentially transport excitons to the heterointerface, where efficient exciton dissociation may occur. However, FRET also competes with charge transfer at the heterointerface turning it in a potential loss mechanism. An energy cascade comprising both energy transfer and charge transfer may aid in separating charges and is briefly discussed. Considering the extent to which the photo-electron conversion efficiency is governed by energy transfer, optimisation of this process offers the prospect of improved organic photovoltaic performance and thus aids in realising the potential of organic solar cells.

Modelling excitonic energy transfer in the photosynthetic unit of purple bacteria

International Nuclear Information System (INIS)

Linnanto, J.M.; Korppi-Tommola, J.E.I.

2009-01-01

Molecular mechanics and quantum chemical configuration interaction calculations in combination with exciton theory were used to predict vibronic energies and eigenstates of light harvesting antennae and the reaction centre and to evaluate excitation energy transfer rates in the photosynthetic unit of purple bacteria. Excitation energy transfer rates were calculated by using the transition matrix formalism and exciton basis sets of the interacting antenna systems. Energy transfer rates of 600-800 fs from B800 ring to B850 ring in the LH2 antenna, 3-10 ps from LH2 to LH2 antenna, 2-8 ps from LH2 to LH1 antenna and finally 30-70 ps from LH1 to the reaction centre were obtained. Dependencies of energy transfer rates on lateral and vertical inter-complex distances were determined. The results indicate that a fair amount of spatial heterogeneity of antenna complexes in the photosynthetic membrane is tolerated without much loss in excitation energy transfer efficiency

Modelling excitonic energy transfer in the photosynthetic unit of purple bacteria

Energy Technology Data Exchange (ETDEWEB)

Linnanto, J.M. [Department of Chemistry, P.O. Box 35, FIN-40014 University of Jyvaeskylae, Jyvaeskylae (Finland)], E-mail: juha.m.linnanto@jyu.fi; Korppi-Tommola, J.E.I. [Department of Chemistry, P.O. Box 35, FIN-40014 University of Jyvaeskylae, Jyvaeskylae (Finland)

2009-02-23

Molecular mechanics and quantum chemical configuration interaction calculations in combination with exciton theory were used to predict vibronic energies and eigenstates of light harvesting antennae and the reaction centre and to evaluate excitation energy transfer rates in the photosynthetic unit of purple bacteria. Excitation energy transfer rates were calculated by using the transition matrix formalism and exciton basis sets of the interacting antenna systems. Energy transfer rates of 600-800 fs from B800 ring to B850 ring in the LH2 antenna, 3-10 ps from LH2 to LH2 antenna, 2-8 ps from LH2 to LH1 antenna and finally 30-70 ps from LH1 to the reaction centre were obtained. Dependencies of energy transfer rates on lateral and vertical inter-complex distances were determined. The results indicate that a fair amount of spatial heterogeneity of antenna complexes in the photosynthetic membrane is tolerated without much loss in excitation energy transfer efficiency.

Energy transfer mechanisms in layered 2D perovskites.

Science.gov (United States)

Williams, Olivia F; Guo, Zhenkun; Hu, Jun; Yan, Liang; You, Wei; Moran, Andrew M

2018-04-07

Two-dimensional (2D) perovskite quantum wells are generating broad scientific interest because of their potential for use in optoelectronic devices. Recently, it has been shown that layers of 2D perovskites can be grown in which the average thicknesses of the quantum wells increase from the back to the front of the film. This geometry carries implications for light harvesting applications because the bandgap of a quantum well decreases as its thickness increases. The general structural formula for the 2D perovskite systems under investigation in this work is (PEA) 2 (MA) n-1 [Pb n I 3n+1 ] (PEA = phenethyl ammonium, MA = methyl ammonium). Here, we examine two layered 2D perovskites with different distributions of quantum well thicknesses. Spectroscopic measurements and model calculations suggest that both systems funnel electronic excitations from the back to the front of the film through energy transfer mechanisms on the time scales of 100's of ps (i.e., energy transfer from thinner to thicker quantum wells). In addition, the model calculations demonstrate that the transient absorption spectra are composed of a progression of single exciton and biexciton resonances associated with the individual quantum wells. We find that exciton dissociation and/or charge transport dynamics make only minor contributions to the transient absorption spectra within the first 1 ns after photo-excitation. An analysis of the energy transfer kinetics indicates that the transitions occur primarily between quantum wells with values of n that differ by 1 because of the spectral overlap factor that governs the energy transfer rate. Two-dimensional transient absorption spectra reveal a pattern of resonances consistent with the dominance of sequential energy transfer dynamics.

Energy transfer mechanisms in layered 2D perovskites

Science.gov (United States)

Williams, Olivia F.; Guo, Zhenkun; Hu, Jun; Yan, Liang; You, Wei; Moran, Andrew M.

2018-04-01

Two-dimensional (2D) perovskite quantum wells are generating broad scientific interest because of their potential for use in optoelectronic devices. Recently, it has been shown that layers of 2D perovskites can be grown in which the average thicknesses of the quantum wells increase from the back to the front of the film. This geometry carries implications for light harvesting applications because the bandgap of a quantum well decreases as its thickness increases. The general structural formula for the 2D perovskite systems under investigation in this work is (PEA)2(MA)n-1[PbnI3n+1] (PEA = phenethyl ammonium, MA = methyl ammonium). Here, we examine two layered 2D perovskites with different distributions of quantum well thicknesses. Spectroscopic measurements and model calculations suggest that both systems funnel electronic excitations from the back to the front of the film through energy transfer mechanisms on the time scales of 100's of ps (i.e., energy transfer from thinner to thicker quantum wells). In addition, the model calculations demonstrate that the transient absorption spectra are composed of a progression of single exciton and biexciton resonances associated with the individual quantum wells. We find that exciton dissociation and/or charge transport dynamics make only minor contributions to the transient absorption spectra within the first 1 ns after photo-excitation. An analysis of the energy transfer kinetics indicates that the transitions occur primarily between quantum wells with values of n that differ by 1 because of the spectral overlap factor that governs the energy transfer rate. Two-dimensional transient absorption spectra reveal a pattern of resonances consistent with the dominance of sequential energy transfer dynamics.

Revealing the ultrafast charge carrier dynamics in organo metal halide perovskite solar cell materials using time resolved THz spectroscopy

Science.gov (United States)

Ponseca, C. S., Jr.; Sundström, V.

2016-03-01

Ultrafast charge carrier dynamics in organo metal halide perovskite has been probed using time resolved terahertz (THz) spectroscopy (TRTS). Current literature on its early time characteristics is unanimous: sub-ps charge carrier generation, highly mobile charges and very slow recombination rationalizing the exceptionally high power conversion efficiency for a solution processed solar cell material. Electron injection from MAPbI3 to nanoparticles (NP) of TiO2 is found to be sub-ps while Al2O3 NPs do not alter charge dynamics. Charge transfer to organic electrodes, Spiro-OMeTAD and PCBM, is sub-ps and few hundreds of ps respectively, which is influenced by the alignment of energy bands. It is surmised that minimizing defects/trap states is key in optimizing charge carrier extraction from these materials.

Continuum model of non-equilibrium solvation and solvent effect on ultra-fast processes

International Nuclear Information System (INIS)

Li Xiangyuan; Fu Kexiang; Zhu Quan

2006-01-01

In the past 50 years, non-equilibrium solvation theory for ultra-fast processes such as electron transfer and light absorption/emission has attracted particular interest. A great deal of research efforts was made in this area and various models which give reasonable qualitative descriptions for such as solvent reorganization energy in electron transfer and spectral shift in solution, were developed within the framework of continuous medium theory. In a series of publications by the authors, we clarified that the expression of the non-equilibrium electrostatic free energy that is at the dominant position of non-equilibrium solvation and serves as the basis of various models, however, was incorrectly formulated. In this work, the authors argue that reversible charging work integration was inappropriately applied in the past to an irreversible path linking the equilibrium or the non-equilibrium state. Because the step from the equilibrium state to the nonequilibrium state is factually thermodynamically irreversible, the conventional expression for non-equilibrium free energy that was deduced in different ways is unreasonable. Here the authors derive the non-equilibrium free energy to a quite different form according to Jackson integral formula. Such a difference throws doubts to the models including the famous Marcus two-sphere model for solvent reorganization energy of electron transfer and the Lippert-Mataga equation for spectral shift. By introducing the concept of 'spring energy' arising from medium polarizations, the energy constitution of the non-equilibrium state is highlighted. For a solute-solvent system, the authors separate the total electrostatic energy into different components: the self-energies of solute charge and polarized charge, the interaction energy between them and the 'spring energy' of the solvent polarization. With detailed reasoning and derivation, our formula for non-equilibrium free energy can be reached through different ways. Based on the

Integrated light in direct excitation and energy transfer luminescence

OpenAIRE

Chimczak, Eugeniusz

2007-01-01

Integrated light in direct excitation and energy transfer luminescence has been investigated. In the investigations reported here, monomolecular centers were taken into account. It was found that the integrated light is equal to the product of generation rate and time of duration of excitation pulse for both direct excitation and energy transfer luminescence.

Energy cascades, excited state dynamics, and photochemistry in cob(III)alamins and ferric porphyrins.

Science.gov (United States)

Rury, Aaron S; Wiley, Theodore E; Sension, Roseanne J

2015-03-17

Porphyrins and the related chlorins and corrins contain a cyclic tetrapyrrole with the ability to coordinate an active metal center and to perform a variety of functions exploiting the oxidation state, reactivity, and axial ligation of the metal center. These compounds are used in optically activated applications ranging from light harvesting and energy conversion to medical therapeutics and photodynamic therapy to molecular electronics, spintronics, optoelectronic thin films, and optomagnetics. Cobalt containing corrin rings extend the range of applications through photolytic cleavage of a unique axial carbon-cobalt bond, permitting spatiotemporal control of drug delivery. The photochemistry and photophysics of cyclic tetrapyrroles are controlled by electronic relaxation dynamics including internal conversion and intersystem crossing. Typically the electronic excitation cascades through ring centered ππ* states, ligand to metal charge transfer (LMCT) states, metal to ligand charge transfer (MLCT) states, and metal centered states. Ultrafast transient absorption spectroscopy provides a powerful tool for the investigation of the electronic state dynamics in metal containing tetrapyrroles. The UV-visible spectrum is sensitive to the oxidation state, electronic configuration, spin state, and axial ligation of the central metal atom. Ultrashort broadband white light probes spanning the range from 270 to 800 nm, combined with tunable excitation pulses, permit the detailed unravelling of the time scales involved in the electronic energy cascade. State-of-the-art theoretical calculations provide additional insight required for precise assignment of the states. In this Account, we focus on recent ultrafast transient absorption studies of ferric porphyrins and corrin containing cob(III)alamins elucidating the electronic states responsible for ultrafast energy cascades, excited state dynamics, and the resulting photoreactivity or photostability of these compounds. Iron

Energy Transfer Kinetics and Dynamics of Relevance to Iodine Lasers

National Research Council Canada - National Science Library

Heaven, Michael C

2001-01-01

...). Energy transfer between I(2 P(1/2)) and 02(X) has been studied in detail. Rate constants for electronic energy transfer and nuclear spin relaxation were measured over the temperature range from 150-300K...

Ultra-fast relaxation, decoherence, and localization of photoexcited states in π-conjugated polymers

Science.gov (United States)

Mannouch, Jonathan R.; Barford, William; Al-Assam, Sarah

2018-01-01

The exciton relaxation dynamics of photoexcited electronic states in poly(p-phenylenevinylene) are theoretically investigated within a coarse-grained model, in which both the exciton and nuclear degrees of freedom are treated quantum mechanically. The Frenkel-Holstein Hamiltonian is used to describe the strong exciton-phonon coupling present in the system, while external damping of the internal nuclear degrees of freedom is accounted for by a Lindblad master equation. Numerically, the dynamics are computed using the time evolving block decimation and quantum jump trajectory techniques. The values of the model parameters physically relevant to polymer systems naturally lead to a separation of time scales, with the ultra-fast dynamics corresponding to energy transfer from the exciton to the internal phonon modes (i.e., the C-C bond oscillations), while the longer time dynamics correspond to damping of these phonon modes by the external dissipation. Associated with these time scales, we investigate the following processes that are indicative of the system relaxing onto the emissive chromophores of the polymer: (1) Exciton-polaron formation occurs on an ultra-fast time scale, with the associated exciton-phonon correlations present within half a vibrational time period of the C-C bond oscillations. (2) Exciton decoherence is driven by the decay in the vibrational overlaps associated with exciton-polaron formation, occurring on the same time scale. (3) Exciton density localization is driven by the external dissipation, arising from "wavefunction collapse" occurring as a result of the system-environment interactions. Finally, we show how fluorescence anisotropy measurements can be used to investigate the exciton decoherence process during the relaxation dynamics.

Photophysical properties and energy transfer mechanism of PFO/Fluorol 7GA hybrid thin films

Energy Technology Data Exchange (ETDEWEB)

Al-Asbahi, Bandar Ali, E-mail: alasbahibandar@gmail.com [School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia); Department of Physics, Faculty of Science, Sana' a University (Yemen); Jumali, Mohammad Hafizuddin Haji, E-mail: hafizhj@ukm.my [School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia); Yap, Chi Chin; Flaifel, Moayad Husein [School of Applied Physics, Faculty of Science and Technology, Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia); Salleh, Muhamad Mat [Institute of Microengineering and Nanoelectronics (IMEN), Universiti Kebangsaan Malaysia (UKM), 43600 Bangi, Selangor (Malaysia)

2013-10-15

Photophysical properties of poly (9,9′-di-n-octylfluorenyl-2.7-diyl) (PFO)/2-butyl-6- (butylamino)benzo [de] isoquinoline-1,3-dione (Fluorol 7GA) and energy transfer between them have been investigated. In this work, both PFO and Fluorol 7GA act as donor and acceptor, respectively. Based on the absorption and luminescence measurements, the photophysical and energy transfer properties such as fluorescence quantum yield (Φ{sub f}), fluorescence lifetime (τ), radiative rate constant (k{sub r}), non-radiative rate constant (k{sub nr}), quenching rate constant (k{sub SV}), energy transfer rate constant (k{sub ET}), energy transfer probability (P{sub DA}), energy transfer efficiency (η), critical concentration of acceptor (C{sub o}), energy transfer time (τ{sub ET}) and critical distance of energy transfer (R{sub o}) were calculated. Large values of k{sub SV}, k{sub ET} and R{sub o} suggested that Förster-type energy transfer was the dominant mechanism for the energy transfer between the excited donor and ground state acceptor molecules. It was observed that the Förster energy transfer together with the trapping process are crucial for performance improvement in ITO/(PFO/Fluorol7GA)/Al device. -- Highlights: • The efficient of energy transfer from PFO to Fluorol 7GA was evidenced. • The resonance energy transfer (Förster type) is the dominant mechanism. • Hsu et al. model was used to calculate Φ{sub f}, τ, k{sub r} and k{sub nr} of PFO thin film. • Several of the photophysical and energy transfer properties were calculated. • Trapping process and Förster energy transfer led to improve the device performance.

Energy transfer processes in Er-doped crystals

International Nuclear Information System (INIS)

Georgescu, Serban; Toma, Octavian

2005-01-01

In this paper, the microparameters characteristic to various energy-transfer processes in erbium doped crystals are estimated using the Dexter theory. For all the investigated processes, electric dipole-dipole interaction between donor and acceptor ions is assumed. The spectra appearing in Dexter's expression of the microparameter are simulated as a superposition of Lorentzian lines, knowing the positions of both initial and final Stark levels, and calibrated using the Judd-Ofelt model. This approach can give an estimation of the importance of the energy-transfer processes. (copyright 2005 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

Chirality and energy transfer amplified circularly polarized luminescence in composite nanohelix

Science.gov (United States)

Yang, Dong; Duan, Pengfei; Zhang, Li; Liu, Minghua

2017-01-01

Transfer of both chirality and energy information plays an important role in biological systems. Here we show a chiral donor π-gelator and assembled it with an achiral π-acceptor to see how chirality and energy can be transferred in a composite donor–acceptor system. It is found that the individual chiral gelator can self-assemble into nanohelix. In the presence of the achiral acceptor, the self-assembly can also proceed and lead to the formation of the composite nanohelix. In the composite nanohelix, an energy transfer is realized. Interestingly, in the composite nanohelix, the achiral acceptor can both capture the supramolecular chirality and collect the circularly polarized energy from the chiral donor, showing both supramolecular chirality and energy transfer amplified circularly polarized luminescence (ETACPL). PMID:28585538

A chopper circuit for energy transfer between superconducting magnets

International Nuclear Information System (INIS)

Onishi, Toshitada; Tateishi, Hiroshi; Takeda, Masatoshi; Matsuura, Toshiaki; Nakatani, Toshio.

1986-01-01

It has been suggested that superconducting magnets could provide a medium for storing energy and supplying the large energy pulses needed by experimental nuclear-fusion equipment and similar loads. Based on this concept, tests on energy transfer between superconducting magnets are currently being conducted at the Agency of Industrial Science and Technology's Electrotechnical Laboratory. Mitsubishi Electric has pioneered the world's first chopper circuit for this application. The circuit has the advantages of being simple and permitting high-speed, bipolar energy transfer. The article describes this circuit and its testing. (author)

Crossed-beam energy transfer: polarization effects and evidence of saturation

Science.gov (United States)

Turnbull, D.; Colaïtis, A.; Follett, R. K.; Palastro, J. P.; Froula, D. H.; Michel, P.; Goyon, C.; Chapman, T.; Divol, L.; Kemp, G. E.; Mariscal, D.; Patankar, S.; Pollock, B. B.; Ross, J. S.; Moody, J. D.; Tubman, E. R.; Woolsey, N. C.

2018-05-01

Recent results on crossed-beam energy transfer are presented. Wavelength tuning was used to vary the amount of energy transfer between two beams in a quasi-stationary plasma with carefully controlled conditions. The amount of transfer agreed well with calculations assuming linear ion acoustic waves (IAWs) with amplitudes up to δ n/n≈ 0.015. Increasing the initial probe intensity to access larger IAW amplitudes for otherwise fixed conditions yields evidence of saturation. The ability to manipulate a beam's polarization, which results from the anisotropic nature of the interaction, is revisited; an example is provided to demonstrate how polarization effects in a multibeam situation can dramatically enhance the expected amount of energy transfer.

Production and transfer of energy and information in Hamiltonian systems.

Directory of Open Access Journals (Sweden)

Chris G Antonopoulos

Full Text Available We present novel results that relate energy and information transfer with sensitivity to initial conditions in chaotic multi-dimensional Hamiltonian systems. We show the relation among Kolmogorov-Sinai entropy, Lyapunov exponents, and upper bounds for the Mutual Information Rate calculated in the Hamiltonian phase space and on bi-dimensional subspaces. Our main result is that the net amount of transfer from kinetic to potential energy per unit of time is a power-law of the upper bound for the Mutual Information Rate between kinetic and potential energies, and also a power-law of the Kolmogorov-Sinai entropy. Therefore, transfer of energy is related with both transfer and production of information. However, the power-law nature of this relation means that a small increment of energy transferred leads to a relatively much larger increase of the information exchanged. Then, we propose an "experimental" implementation of a 1-dimensional communication channel based on a Hamiltonian system, and calculate the actual rate with which information is exchanged between the first and last particle of the channel. Finally, a relation between our results and important quantities of thermodynamics is presented.

2013 MOLECULAR ENERGY TRANSFER GORDON RESEARCH CONFERENCE (JANUARY 13-18, 2013 - VENTURA BEACH MARRIOTT, VENTURA CA

Energy Technology Data Exchange (ETDEWEB)

Reid, Scott A. [Marquette University

2012-10-18

Sessions covered all areas of molecular energy transfer, with 10 sessions of talks and poster sessions covering the areas of :  Energy Transfer in Inelastic and Reactive Scattering  Energy Transfer in Photoinitiated and Unimolecular Reactions  Non-adiabatic Effects in Energy Transfer  Energy Transfer at Surfaces and Interfaces  Energy Transfer in Clusters, Droplets, and Aerosols  Energy Transfer in Solution and Solid  Energy Transfer in Complex Systems  Energy Transfer: New vistas and horizons  Molecular Energy Transfer: Where Have We Been and Where are We Going?

Interaction mechanism for energy transfer from Ce to Tb ions in silica

International Nuclear Information System (INIS)

Seed Ahmed, H.A.A.; Chae, W.S.; Ntwaeaborwa, O.M.; Kroon, R.E.

2016-01-01

Energy transfer phenomena can play an important role in the development of luminescent materials. In this study, numerical simulations based on theoretical models of non-radiative energy transfer are compared to experimental results for Ce, Tb co-doped silica. Energy transfer from the donor (Ce) to the acceptor (Tb) resulted in a decrease in the Ce luminescence intensity and lifetime. The decrease in intensity corresponded best with the energy transfer models based on the exchange interaction and the dipole-dipole interaction. The critical transfer distance obtained from the fitting using both these models is around 2 nm. Since the exchange interaction requires a distance shorter than 1 nm to occur, the mechanism most likely to account for the energy transfer is concluded to be the dipole–dipole interaction. This is supported by an analysis of the lifetime data.

Modeling of MeV alpha particle energy transfer to lower hybrid waves

International Nuclear Information System (INIS)

Schivell, J.; Monticello, D.A.; Fisch, N.; Rax, J.M.

1993-10-01

The interaction between a lower hybrid wave and a fusion alpha particle displaces the alpha particle simultaneously in space and energy. This results in coupled diffusion. Diffusion of alphas down the density gradient could lead to their transferring energy to the wave. This could, in turn, put energy into current drive. An initial analytic study was done by Fisch and Rax. Here the authors calculate numerical solutions for the alpha energy transfer and study a range of conditions that are favorable for wave amplification from alpha energy. They find that it is possible for fusion alpha particles to transfer a large fraction of their energy to the lower hybrid wave. The numerical calculation shows that the net energy transfer is not sensitive to the value of the diffusion coefficient over a wide range of practical values. An extension of this idea, the use of a lossy boundary to enhance the energy transfer, is investigated. This technique is shown to offer a large potential benefit

Reversible ultrafast melting in bulk CdSe

International Nuclear Information System (INIS)

Wu, Wenzhi; He, Feng; Wang, Yaguo

2016-01-01

In this work, transient reflectivity changes in bulk CdSe have been measured with two-color femtosecond pump-probe spectroscopy under a wide range of pump fluences. Three regions of reflectivity change with pump fluences have been consistently revealed for excited carrier density, coherent phonon amplitude, and lattice temperature. For laser fluences from 13 to 19.3 mJ/cm 2 , ultrafast melting happens in first several picoseconds. This melting process is purely thermal and reversible. A complete phase transformation in bulk CdSe may be reached when the absorbed laser energy is localized long enough, as observed in nanocrystalline CdSe

Multi-step intramolecular excitation energy transfer in dendritic pyrene-phosphorus(V)porphyrin heptads

Energy Technology Data Exchange (ETDEWEB)

Hirakawa, Kazutaka, E-mail: hirakawa.kazutaka@shizuoka.ac.jp [Applied Chemistry and Biochemical Engineering Course, Department of Engineering, Graduate School of Integrated Science and Technology, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561 (Japan); Department of Optoelectronics and Nanostructure Science, Graduate School of Science and Technology, Shizuoka University, Johoku 3-5-1, Naka-ku, Hamamatsu, Shizuoka 432-8561 (Japan); Segawa, Hiroshi [Department of Multi-Disciplinary Science - General Systems Studies, Graduate School of Arts and Sciences, The University of Tokyo, Komaba 3-8-1, Meguro-ku, Tokyo 153-8904 (Japan); Research Center for Advanced Science and Technology, The University of Tokyo, Komaba 4-6-1, Meguro-ku, Tokyo 153-8904 (Japan)

2016-11-15

Dendritic heptad molecules in which four pyrenyl groups are connected at the central phosphorus atom of the edge-porphyrins of the center-to-edge type porphyrin trimers were synthesized to investigate a multi-step excitation energy transfer. As the central energy acceptor, two types porphyrins which one was phosphorus(V)tetraphenylporphyrin (H2) and another was its derivative substituted by butoxy groups at four para-position of meso-phenyl groups (H1) were used. In the photoexcited state of the pyrene units, the excitation energy transfer to the central-porphyrin unit was observed in toluene. The excitation energy transfer is considered to be through two pathways; one is a stepwise pathway through the edge-porphyrin unit and another is a direct excitation energy transfer to the central porphyrin. The direct excitation energy transfer from pyrenes to the edge-porphyrin and central-porphyrin were observed in the case for H1. From the excited state of the edge-porphyrins, the excitation energy transfer to the central-porphyrin occurs in the H1 case. In the H2 case, the excitation energy of central-porphyrin is higher than that of H1, and the electron transfer from edge-porphyrin to the central-porphyrin become predominant process. - Highlights: • Dendritic pyrene-porphyrin heptads were synthesized. • Excitation energy transfer occurs from the pyrenyl moiety to the phosphorus(V)porphyrin. • The stepwise and direct energy transfer pathways were observed. • The quantum yields of these energy transfer pathways could be determined.

Multi-step intramolecular excitation energy transfer in dendritic pyrene-phosphorus(V)porphyrin heptads

International Nuclear Information System (INIS)

Hirakawa, Kazutaka; Segawa, Hiroshi

2016-01-01

Dendritic heptad molecules in which four pyrenyl groups are connected at the central phosphorus atom of the edge-porphyrins of the center-to-edge type porphyrin trimers were synthesized to investigate a multi-step excitation energy transfer. As the central energy acceptor, two types porphyrins which one was phosphorus(V)tetraphenylporphyrin (H2) and another was its derivative substituted by butoxy groups at four para-position of meso-phenyl groups (H1) were used. In the photoexcited state of the pyrene units, the excitation energy transfer to the central-porphyrin unit was observed in toluene. The excitation energy transfer is considered to be through two pathways; one is a stepwise pathway through the edge-porphyrin unit and another is a direct excitation energy transfer to the central porphyrin. The direct excitation energy transfer from pyrenes to the edge-porphyrin and central-porphyrin were observed in the case for H1. From the excited state of the edge-porphyrins, the excitation energy transfer to the central-porphyrin occurs in the H1 case. In the H2 case, the excitation energy of central-porphyrin is higher than that of H1, and the electron transfer from edge-porphyrin to the central-porphyrin become predominant process. - Highlights: • Dendritic pyrene-porphyrin heptads were synthesized. • Excitation energy transfer occurs from the pyrenyl moiety to the phosphorus(V)porphyrin. • The stepwise and direct energy transfer pathways were observed. • The quantum yields of these energy transfer pathways could be determined.

Laser selective cutting of biological tissues by impulsive heat deposition through ultrafast vibrational excitations.

Science.gov (United States)

Franjic, Kresimir; Cowan, Michael L; Kraemer, Darren; Miller, R J Dwayne

2009-12-07

Mechanical and thermodynamic responses of biomaterials after impulsive heat deposition through vibrational excitations (IHDVE) are investigated and discussed. Specifically, we demonstrate highly efficient ablation of healthy tooth enamel using 55 ps infrared laser pulses tuned to the vibrational transition of interstitial water and hydroxyapatite around 2.95 microm. The peak intensity at 13 GW/cm(2) was well below the plasma generation threshold and the applied fluence 0.75 J/cm(2) was significantly smaller than the typical ablation thresholds observed with nanosecond and microsecond pulses from Er:YAG lasers operating at the same wavelength. The ablation was performed without adding any superficial water layer at the enamel surface. The total energy deposited per ablated volume was several times smaller than previously reported for non-resonant ultrafast plasma driven ablation with similar pulse durations. No micro-cracking of the ablated surface was observed with a scanning electron microscope. The highly efficient ablation is attributed to an enhanced photomechanical effect due to ultrafast vibrational relaxation into heat and the scattering of powerful ultrafast acoustic transients with random phases off the mesoscopic heterogeneous tissue structures.

Ultrafast Bessel beams: advanced tools for laser materials processing

Science.gov (United States)

Stoian, Razvan; Bhuyan, Manoj K.; Zhang, Guodong; Cheng, Guanghua; Meyer, Remy; Courvoisier, Francois

2018-05-01

Ultrafast Bessel beams demonstrate a significant capacity of structuring transparent materials with a high degree of accuracy and exceptional aspect ratio. The ability to localize energy on the nanometer scale (bypassing the 100-nm milestone) makes them ideal tools for advanced laser nanoscale processing on surfaces and in the bulk. This allows to generate and combine micron and nano-sized features into hybrid structures that show novel functionalities. Their high aspect ratio and the accurate location can equally drive an efficient material modification and processing strategy on large dimensions. We review, here, the main concepts of generating and using Bessel non-diffractive beams and their remarkable features, discuss general characteristics of their interaction with matter in ablation and material modification regimes, and advocate their use for obtaining hybrid micro and nanoscale structures in two and three dimensions (2D and 3D) performing complex functions. High-throughput applications are indicated. The example list ranges from surface nanostructuring and laser cutting to ultrafast laser welding and the fabrication of 3D photonic systems embedded in the volume.

A US Based Ultrafast Interdisciplinary Research Facility

Science.gov (United States)

Gueye, Paul; Hill, Wendell; Johnson, Anthony

2006-10-01

The US scientific competitiveness on the world arena has substantially decreased due to the lack of funding and training of qualified personnel. Most of the potential workforce found in higher education is composed of foreign students and post-docs. In the specific field of low- and high-field science, the European and Asian communities are rapidly catching-up with the US, even leading in some areas. To remain the leader in ultrafast science and technology, new visions and commitment must be embraced. For that reason, an international effort of more than 70 countries for a US-based interdisciplinary research facility using ultrafast laser technology is under development. It will provide research and educational training, as well as new venues for a strong collaboration between the fields of astrophysics, nuclear/high energy physics, plasma physics, optical sciences, biological and medical physics. This facility will consist of a uniquely designed high contrast multi-lines concept housing twenty experimental rooms shared between four beams:[0.1 TW, 1 kHz], [10 TW, 9 kHz], [100-200 TW, 10 Hz] and [500 TW, 10 Hz]. The detail schematic of this multi-laser system, foreseen research and educational programs, and organizational structure of this facility will be presented.

Role of coherence and delocalization in photo-induced electron transfer at organic interfaces

Science.gov (United States)

Abramavicius, V.; Pranculis, V.; Melianas, A.; Inganäs, O.; Gulbinas, V.; Abramavicius, D.

2016-09-01

Photo-induced charge transfer at molecular heterojunctions has gained particular interest due to the development of organic solar cells (OSC) based on blends of electron donating and accepting materials. While charge transfer between donor and acceptor molecules can be described by Marcus theory, additional carrier delocalization and coherent propagation might play the dominant role. Here, we describe ultrafast charge separation at the interface of a conjugated polymer and an aggregate of the fullerene derivative PCBM using the stochastic Schrödinger equation (SSE) and reveal the complex time evolution of electron transfer, mediated by electronic coherence and delocalization. By fitting the model to ultrafast charge separation experiments, we estimate the extent of electron delocalization and establish the transition from coherent electron propagation to incoherent hopping. Our results indicate that even a relatively weak coupling between PCBM molecules is sufficient to facilitate electron delocalization and efficient charge separation at organic interfaces.

Optical absorption and energy transfer processes in dendrimers

International Nuclear Information System (INIS)

Reineker, P.; Engelmann, A.; Yudson, V.I.

2004-01-01

For dendrimers of various sizes the energy transfer and the optical absorption is investigated theoretically. The molecular subunits of a dendrimer are modeled as two-level systems. The electronic interaction between them is described via transfer integrals and the influence of vibrational degrees of freedom is taken into account in a first approach using a stochastic model. We discuss the time dependence of the energy transport and show that rim states of the dendrimer dominate the absorption spectra, that in general the electronic excitation energy is concentrated on peripheric molecules, and that the energetically lowest absorption peak is redshifted with increasing dendrimer size due to delocalization of the electronic excitation

State-of-the-Art Developments of Acoustic Energy Transfer

Directory of Open Access Journals (Sweden)

Md Rabiul Awal

2016-01-01

Full Text Available Acoustic energy transfer (AET technology has drawn significant industrial attention recently. This paper presents the reviews of the existing AETs sequentially, preferably, from the early stage. From the review, it is evident that, among all the classes of wireless energy transfer, AET is the safest technology to adopt. Thus, it is highly recommended for sensitive area and devices, especially implantable devices. Though, the efficiency for relatively long distances (i.e., >30 mm is less than that of inductive or capacitive power transfer; however, the trade-off between safety considerations and performances is highly suitable and better than others. From the presented statistics, it is evident that AET is capable of transmitting 1.068 kW and 5.4 W of energy through wall and in-body medium (implants, respectively. Progressively, the AET efficiency can reach up to 88% in extension to 8.6 m separation distance which is even superior to that of inductive and capacitive power transfer.

Subwavelength dielectric nanorod chains for energy transfer in the visible range.

Science.gov (United States)

Li, Dongdong; Zhang, Jingjing; Yan, Changchun; Xu, Zhengji; Zhang, Dao Hua

2017-10-15

We report a new type of energy transfer device, formed by a dielectric nanorod array embedded in a silver slab. Such dielectric chain structures allow surface plasmon wave guiding with large propagation length and highly suppressed crosstalk between adjacent transmission channels. The simulation results show that our proposed design can be used to enhance the energy transfer along the waveguide-like dielectric nanorod chains via coupled plasmons, where the energy spreading is effectively suppressed, and superior imaging properties in terms of resolution and energy transfer distance can be achieved.

Electron transfer in organic glass. Distance and energy dependence

International Nuclear Information System (INIS)

Krongauz, V.V.

1992-01-01

The authors have investigated the distance and energy dependence of electron transfer in rigid organic glasses containing randomly dispersed electron donor and electron acceptor molecules. Pulsed radiolysis by an electron beam from a linear accelerator was used for ionization resulting in charge deposition on donor molecules. The disappearance kinetics of donor radical anions due to electron transfer to acceptor was monitored spectroscopically by the change in optical density at the wavelength corresponding to that of donor radical anion absorbance. It was found that the rate of the electron transfer observed experimentally was higher than that computed using the Marcus-Levich theory assuming that the electron-transfer activation barrier is equal to the binding energy of electron on the donor molecule. This discrepancy between the experimental and computed results suggests that the open-quotes inertclose quotes media in which electron-transfer reaction takes place may be participating in the process, resulting in experimentally observed higher electron-transfer rates. 32 refs., 3 figs., 2 tabs

Nanophotonic Control of the Förster Resonance Energy Transfer Efficiency

DEFF Research Database (Denmark)

Blum, Christian; Zijlstra, Niels; Lagendijk, Ad

2012-01-01

We have studied the influence of the local density of optical states (LDOS) on the rate and efficiency of Forster resonance energy transfer (FRET) from a donor to an acceptor. The donors and acceptors are dye molecules that are separated by a short strand of double-stranded DNA. The LDOS...... is controlled by carefully positioning the FRET pairs near a mirror. We find that the energy transfer efficiency changes with LDOS, and that, in agreement with theory, the energy transfer rate is independent of the LDOS, which allows one to quantitatively control FRET systems in a new way. Our results imply...

Single-Molecule Interfacial Electron Transfer

Energy Technology Data Exchange (ETDEWEB)

Lu, H. Peter [Bowling Green State Univ., Bowling Green, OH (United States). Dept. of Chemistry and Center for Photochemical Sciences

2017-11-28

This project is focused on the use of single-molecule high spatial and temporal resolved techniques to study molecular dynamics in condensed phase and at interfaces, especially, the complex reaction dynamics associated with electron and energy transfer rate processes. The complexity and inhomogeneity of the interfacial ET dynamics often present a major challenge for a molecular level comprehension of the intrinsically complex systems, which calls for both higher spatial and temporal resolutions at ultimate single-molecule and single-particle sensitivities. Combined single-molecule spectroscopy and electrochemical atomic force microscopy approaches are unique for heterogeneous and complex interfacial electron transfer systems because the static and dynamic inhomogeneities can be identified and characterized by studying one molecule at a specific nanoscale surface site at a time. The goal of our project is to integrate and apply these spectroscopic imaging and topographic scanning techniques to measure the energy flow and electron flow between molecules and substrate surfaces as a function of surface site geometry and molecular structure. We have been primarily focusing on studying interfacial electron transfer under ambient condition and electrolyte solution involving both single crystal and colloidal TiO₂ and related substrates. The resulting molecular level understanding of the fundamental interfacial electron transfer processes will be important for developing efficient light harvesting systems and broadly applicable to problems in fundamental chemistry and physics. We have made significant advancement on deciphering the underlying mechanism of the complex and inhomogeneous interfacial electron transfer dynamics in dyesensitized TiO₂ nanoparticle systems that strongly involves with and regulated by molecule-surface interactions. We have studied interfacial electron transfer on TiO₂ nanoparticle surfaces by using ultrafast single

Ultrafast Raman scattering in gas-filled hollow-core fibers

OpenAIRE

Belli, Federico

2017-01-01

The experimental and numerical work reported here is rooted in ultrafast molecular phenomena and nonlinear fiber optics, which are brought together in a deceptively simple system: a homo-nuclear molecular gas (e.g. H2,D2) loaded in the hollow-core of a broad-band guiding photonic crystal fiber (PCF) and exposed to ultrashort pulses of moderate energies (∼ μJ). On one hand, the choice of a molecular gas as the nonlinear medium provides a rich playground for light-matter interactions. ...

A Design Study Of A Wireless Power Transfer System For Use To Transfer Energy From A Vibration Energy Harvester

Science.gov (United States)

Grabham, N. J.; Harden, C.; Vincent, D.; Beeby, S. P.

2016-11-01

A wirelessly powered remote sensor node is presented along with its design process. The purpose of the node is the further expansion of the sensing capabilities of the commercial Perpetuum system used for condition monitoring on trains and rolling stock which operates using vibration energy harvesting. Surplus harvested vibration energy is transferred wirelessly to a remote satellite sensor to allow measurements over a wider area to be made. This additional data is to be used for long term condition monitoring. Performance measurements made on the prototype remote sensor node are reported and advantages and disadvantages of using the same RF frequency for power and data transfer are identified.

Theoretical Study of Ultrafast Electron Injection into a Dye/TiO2 System in Dye-Sensitized Solar Cells

Science.gov (United States)

Lin, Chundan; Xia, Qide; Li, Kuan; Li, Juan; Yang, Zhenqing

2018-06-01

The ultrafast injection of excited electrons in dye/TiO2 system plays a critical role, which determines the device's efficiency in large part. In this work, we studied the geometrical structures and electronic properties of a dye/TiO2 composite system for dye-sensitized solar cells (DSSCs) by using density functional theory, and we analyzed the mechanism of ultrafast electron injection with emphasis on the power conversion efficiency. The results show that the dye SPL103/TiO2 (101) surface is more stable than dye SPL101. The electron injection driving force of SPL103/TiO2 (101) is 3.55 times that of SPL101, indicating that SPL103/TiO2 (101) has a strong ability to transfer electrons. SPL103 and SPL101/TiO2 (101) both have fast electron transfer processes, and especially the electron injection time of SPL103/TiO2 (101) is only 1.875 fs. The results of this work are expected to provide a new understanding of the mechanism of electron injection in dyes/TiO2 systems for use in highly effective DSSCs.

Dependence of adiabatic population transfer on pulse profile

Indian Academy of Sciences (India)

Control of population transfer by rapid adiabatic passage has been an established technique wherein the exact amplitude profile of the shaped pulse is considered to be insignificant. We study the effect of ultrafast shaped pulses for two-level systems, by density-matrix approach. However, we find that adiabaticity depends ...

Excitonic energy transfer in light-harvesting complexes in purple bacteria

International Nuclear Information System (INIS)

Ye Jun; Sun Kewei; Zhao Yang; Lee, Chee Kong; Yu Yunjin; Cao Jianshu

2012-01-01

Two distinct approaches, the Frenkel-Dirac time-dependent variation and the Haken-Strobl model, are adopted to study energy transfer dynamics in single-ring and double-ring light-harvesting (LH) systems in purple bacteria. It is found that the inclusion of long-range dipolar interactions in the two methods results in significant increase in intra- or inter-ring exciton transfer efficiency. The dependence of exciton transfer efficiency on trapping positions on single rings of LH2 (B850) and LH1 is similar to that in toy models with nearest-neighbor coupling only. However, owing to the symmetry breaking caused by the dimerization of BChls and dipolar couplings, such dependence has been largely suppressed. In the studies of coupled-ring systems, both methods reveal an interesting role of dipolar interactions in increasing energy transfer efficiency by introducing multiple intra/inter-ring transfer paths. Importantly, the time scale (4 ps) of inter-ring exciton transfer obtained from polaron dynamics is in good agreement with previous studies. In a double-ring LH2 system, non-nearest neighbor interactions can induce symmetry breaking, which leads to global and local minima of the average trapping time in the presence of a non-zero dephasing rate, suggesting that environment dephasing helps preserve quantum coherent energy transfer when the perfect circular symmetry in the hypothetic system is broken. This study reveals that dipolar coupling between chromophores may play an important role in the high energy transfer efficiency in the LH systems of purple bacteria and many other natural photosynthetic systems.

Excitonic energy transfer in light-harvesting complexes in purple bacteria

Energy Technology Data Exchange (ETDEWEB)

Ye Jun; Sun Kewei; Zhao Yang; Lee, Chee Kong [School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798 (Singapore); Yu Yunjin [School of Materials Science and Engineering, Nanyang Technological University, Singapore 639798 (Singapore); College of Physics Science and Technology, Shenzhen University, Guangdong 518060 (China); Cao Jianshu [Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139 (United States)

2012-06-28

Two distinct approaches, the Frenkel-Dirac time-dependent variation and the Haken-Strobl model, are adopted to study energy transfer dynamics in single-ring and double-ring light-harvesting (LH) systems in purple bacteria. It is found that the inclusion of long-range dipolar interactions in the two methods results in significant increase in intra- or inter-ring exciton transfer efficiency. The dependence of exciton transfer efficiency on trapping positions on single rings of LH2 (B850) and LH1 is similar to that in toy models with nearest-neighbor coupling only. However, owing to the symmetry breaking caused by the dimerization of BChls and dipolar couplings, such dependence has been largely suppressed. In the studies of coupled-ring systems, both methods reveal an interesting role of dipolar interactions in increasing energy transfer efficiency by introducing multiple intra/inter-ring transfer paths. Importantly, the time scale (4 ps) of inter-ring exciton transfer obtained from polaron dynamics is in good agreement with previous studies. In a double-ring LH2 system, non-nearest neighbor interactions can induce symmetry breaking, which leads to global and local minima of the average trapping time in the presence of a non-zero dephasing rate, suggesting that environment dephasing helps preserve quantum coherent energy transfer when the perfect circular symmetry in the hypothetic system is broken. This study reveals that dipolar coupling between chromophores may play an important role in the high energy transfer efficiency in the LH systems of purple bacteria and many other natural photosynthetic systems.

Stochastic Modelling of Wireless Energy Transfer

Science.gov (United States)

Veilleux, Shaun; Almaghasilah, Ahmed; Abedi, Ali; Wilkerson, DeLisa

2017-01-01

This study investigates the efficiency of a new method of powering remote sensors by the means of wireless energy transfer. The increased use of sensors for data collection comes with the inherent cost of supplying power from sources such as power cables or batteries. Wireless energy transfer technology eliminates the need for power cables or periodic battery replacement. The time and cost of setting up or expanding a sensor network will be reduced while allowing sensors to be placed in areas where running power cables or battery replacement is not feasible. This paper models wireless channels for power and data separately. Smart scheduling for the data channel is proposed to avoid transmitting data on a noisy channel where the probability of data loss is high to improve power efficiency. Analytical models have been developed and verified using simulations.

Nonlinear ultrafast optical response in organic molecular crystals

Science.gov (United States)

Rahman, Talat S.; Turkowski, Volodymyr; Leuenberger, Michael N.

2012-02-01

We analyze possible nonlinear excitonic effects in the organic molecule crystals by using a combined time-dependent DFT and many-body approach. In particular, we analyze possible effects of the time-dependent (retarded)interaction between different types of excitations, Frenkel excitons, charge transfer excitons and excimers, on the electric and the optical response of the system. We pay special attention to the case of constant electric field and ultrafast pulses, including that of four-wave mixing experiments. As a specific application we examine the optical excitations of pentacene nanocrystals and compare the results with available experimental data.[1] Our results demostrate that the nonlinear effects can play an important role in the optical response of these systems. [1] A. Kabakchiev, ``Scanning Tunneling Luminescence of Pentacene Nanocrystals'', PhD Thesis (EPFL, Lausanne, 2010).

Theory of pump–probe ultrafast photoemission and X-ray absorption spectra

Energy Technology Data Exchange (ETDEWEB)

Fujikawa, Takashi, E-mail: tfujikawa@faculty.chiba-u.jp; Niki, Kaori

2016-01-15

Highlights: • Pump–probe ultrafast XAFS and XPS spectra are theoretically studied. • Keldysh Green's function theory is applied. • Important many-body effects are explicitly included. - Abstract: Keldysh Green's function approach is extensively used in order to derive practical formulas to analyze pump–probe ultrafast photoemission and X-ray absorption spectra. Here the pump pulse is strong enough whereas the probe X-ray pulse can be treated by use of a perturbation theory. We expand full Green's function in terms of renormalized Green's function without the interaction between electrons and probe pulse. The present theoretical formulas allow us to handle the intrinsic and extrinsic losses, and furthermore resonant effects in X-ray Absorption Fine Structures (XAFS). To understand the radiation field screening in XPS spectra, we have to use more sophisticated theoretical approach. In the ultrafast XPS and XAFS analyses the intrinsic and extrinsic loss effects can interfere as well. In the XAFS studies careful analyses are necessary to handle extrinsic losses in terms of damped photoelectron propagation. The nonequilibrium dynamics after the pump pulse irradiation is well described by use of the time-dependent Dyson orbitals. Well above the edge threshold, ultrafast photoelectron diffraction and extended X-ray absorption fine structure (EXAFS) provide us with transient structural change after the laser pump excitations. In addition to these slow processes, the rapid oscillation in time plays an important role related to pump electronic excitations. Near threshold detailed information could be obtained for the combined electronic and structural dynamics. In particular high-energy photoemission and EXAFS are not so influenced by the details of excited states by pump pulse. Random-Phase Approximation (RPA)-boson approach is introduced to derive some practical formulas for time-dependent intrinsic amplitudes.

Ultrafast generation of pseudo-magnetic field for valley excitons in WSe2 monolayers

KAUST Repository

Kim, J.

2014-12-04

The valley pseudospin is a degree of freedom that emerges in atomically thin two-dimensional transition metal dichalcogenides (MX2). The capability to manipulate it, in analogy to the control of spin in spintronics, can open up exciting opportunities. Here, we demonstrate that an ultrafast and ultrahigh valley pseudo-magnetic field can be generated by using circularly polarized femtosecond pulses to selectively control the valley degree of freedom in monolayer MX2. Using ultrafast pump-probe spectroscopy, we observed a pure and valley-selective optical Stark effect in WSe2 monolayers from the nonresonant pump, resulting in an energy splitting of more than 10 milli-electron volts between the K and K′ valley exciton transitions. Our study opens up the possibility to coherently manipulate the valley polarization for quantum information applications.

Ultrafast generation of pseudo-magnetic field for valley excitons in WSe2 monolayers

KAUST Repository

Kim, J.; Hong, X.; Jin, C.; Shi, S.-F.; Chang, C.-Y. S.; Chiu, Ming-Hui; Li, Lain-Jong; Wang, F.

2014-01-01

The valley pseudospin is a degree of freedom that emerges in atomically thin two-dimensional transition metal dichalcogenides (MX2). The capability to manipulate it, in analogy to the control of spin in spintronics, can open up exciting opportunities. Here, we demonstrate that an ultrafast and ultrahigh valley pseudo-magnetic field can be generated by using circularly polarized femtosecond pulses to selectively control the valley degree of freedom in monolayer MX2. Using ultrafast pump-probe spectroscopy, we observed a pure and valley-selective optical Stark effect in WSe2 monolayers from the nonresonant pump, resulting in an energy splitting of more than 10 milli-electron volts between the K and K′ valley exciton transitions. Our study opens up the possibility to coherently manipulate the valley polarization for quantum information applications.

Ultrafast photoinduced structure phase transition in antimony single crystals

NARCIS (Netherlands)

Fausti, Daniele; Misochko, Oleg V.; van Loosdrecht, Paul H. M.

2009-01-01

Picosecond Raman scattering is used to study the photoinduced ultrafast dynamics in Peierls distorted antimony. We find evidence for an ultrafast nonthermal reversible structural phase transition. Most surprisingly, we find evidence that this transition evolves toward a lower symmetry in contrast to

Graphene-based chemiluminescence resonance energy transfer for homogeneous immunoassay.

Science.gov (United States)

Lee, Joon Seok; Joung, Hyou-Arm; Kim, Min-Gon; Park, Chan Beum

2012-04-24

We report on chemiluminescence resonance energy transfer (CRET) between graphene nanosheets and chemiluminescent donors. In contrast to fluorescence resonance energy transfer, CRET occurs via nonradiative dipole-dipole transfer of energy from a chemiluminescent donor to a suitable acceptor molecule without an external excitation source. We designed a graphene-based CRET platform for homogeneous immunoassay of C-reactive protein (CRP), a key marker for human inflammation and cardiovascular diseases, using a luminol/hydrogen peroxide chemiluminescence (CL) reaction catalyzed by horseradish peroxidase. According to our results, anti-CRP antibody conjugated to graphene nanosheets enabled the capture of CRP at the concentration above 1.6 ng mL(-1). In the CRET platform, graphene played a key role as an energy acceptor, which was more efficient than graphene oxide, while luminol served as a donor to graphene, triggering the CRET phenomenon between luminol and graphene. The graphene-based CRET platform was successfully applied to the detection of CRP in human serum samples in the range observed during acute inflammatory stress.

Progress in ultrafast intense laser science

CERN Document Server

Yamanouchi, Kaoru; Mathur, Deepak

2014-01-01

The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science, and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance

Mechanism and models for collisional energy transfer in highly excited large polyatomic molecules

International Nuclear Information System (INIS)

Gilbert, R. G.

1995-01-01

Collisional energy transfer in highly excited molecules (say, 200-500 kJ mol -1 above the zero-point energy of reactant, or of product, for a recombination reaction) is reviewed. An understanding of this energy transfer is important in predicting and interpreting the pressure dependence of gas-phase rate coefficients for unimolecular and recombination reactions. For many years it was thought that this pressure dependence could be calculated from a single energy-transfer quantity, such as the average energy transferred per collision. However, the discovery of 'super collisions' (a small but significant fraction of collisions which transfer abnormally large amounts of energy) means that this simplistic approach needs some revision. The 'ordinary' (non-super) component of the distribution function for collisional energy transfer can be quantified either by empirical models (e.g., an exponential-down functional form) or by models with a physical basis, such as biased random walk (applicable to monatomic or diatomic collision partners) or ergodic (for polyatomic collision partners) treatments. The latter two models enable approximate expressions for the average energy transfer to be estimated from readily available molecular parameters. Rotational energy transfer, important for finding the pressure dependence for recombination reactions, can for these purposes usually be taken as transferring sufficient energy so that the explicit functional form is not required to predict the pressure dependence. The mechanism of 'ordinary' energy transfer seems to be dominated by low-frequency modes of the substrate, whereby there is sufficient time during a vibrational period for significant energy flow between the collision partners. Super collisions may involve sudden energy flow as an outer atom of the substrate is squashed between the substrate and the bath gas, and then is moved away from the interaction by large-amplitude motion such as a ring vibration or a rotation; improved

Energy transfer of excitons between quantum wells separated by a wide barrier

International Nuclear Information System (INIS)

Lyo, S. K.

2000-01-01

We present a microscopic theory of the excitonic Stokes and anti-Stokes energy-transfer mechanisms between two widely separated unequal quantum wells with a large energy mismatch (Δ) at low temperatures (T). Several important intrinsic energy-transfer mechanisms have been examined, including dipolar coupling, real and virtual photon-exchange coupling, and over-barrier ionization of the excitons via exciton-exciton Auger processes. The transfer rate is calculated as a function of T and the center-to-center distance d between the wells. The rates depend sensitively on T for plane-wave excitons. For localized excitons, the rates depend on T only through the T dependence of the exciton localization radius. For Stokes energy transfer, the dominant energy transfer occurs through a photon-exchange interaction, which enables the excitons from the higher-energy wells to decay into free electrons and holes in the lower-energy wells. The rate has a slow dependence on d, yielding reasonable agreement with recent data from GaAs/Al x Ga 1-x As quantum wells. The dipolar rate is about an order of magnitude smaller for large d (e.g., d=175Aa) with a stronger range dependence proportional to d -4 . However, the latter can be comparable to the radiative rate for small d (e.g., d≤80Aa). For anti-Stokes transfer through exchange-type (e.g., dipolar and photon-exchange) interactions, we show that thermal activation proportional to exp(-Δ/k B T) is essential for the transfer, contradicting a recent nonactivated result based on the Fo''rster-Dexter's spectral-overlap theory. Phonon-assisted transfer yields a negligibly small rate. On the other hand, energy transfer through over-barrier ionization of excitons via Auger processes yields a significantly larger nonactivated rate which is independent of d. The result is compared with recent data

Ultrafast THz Saturable Absorption in Doped Semiconductors

DEFF Research Database (Denmark)

Turchinovich, Dmitry; Hoffmann, Matthias C.

2011-01-01

We demonstrate ultrafast THz saturable absorption in n-doped semiconductors by nonlinear THz time-domain spectroscopy. This effect is caused by the semiconductor conductivity modulation due to electron heating and satellite-valley scattering in strong THz fields.......We demonstrate ultrafast THz saturable absorption in n-doped semiconductors by nonlinear THz time-domain spectroscopy. This effect is caused by the semiconductor conductivity modulation due to electron heating and satellite-valley scattering in strong THz fields....

Concept and design of a beam blanker with integrated photoconductive switch for ultrafast electron microscopy.

Science.gov (United States)

Weppelman, I G C; Moerland, R J; Hoogenboom, J P; Kruit, P

2018-01-01

We present a new method to create ultrashort electron pulses by integrating a photoconductive switch with an electrostatic deflector. This paper discusses the feasibility of such a system by analytical and numerical calculations. We argue that ultrafast electron pulses can be achieved for micrometer scale dimensions of the blanker, which are feasible with MEMS-based fabrication technology. According to basic models, the design presented in this paper is capable of generating 100 fs electron pulses with spatial resolutions of less than 10 nm. Our concept for an ultrafast beam blanker (UFB) may provide an attractive alternative to perform ultrafast electron microscopy, as it does not require modification of the microscope nor realignment between DC and pulsed mode of operation. Moreover, only low laser pulse energies are required. Due to its small dimensions the UFB can be inserted in the beam line of a commercial microscope via standard entry ports for blankers or variable apertures. The use of a photoconductive switch ensures minimal jitter between laser and electron pulses. Copyright © 2017 Elsevier B.V. All rights reserved.

Modeling the efficiency of Förster resonant energy transfer from energy relay dyes in dye-sensitized solar cells

KAUST Repository

Hoke, Eric T.; Hardin, Brian E.; McGehee, Michael D.

2010-01-01

Förster resonant energy transfer can improve the spectral breadth, absorption and energy conversion efficiency of dye sensitized solar cells. In this design, unattached relay dyes absorb the high energy photons and transfer the excitation

Wireless Energy Transfer Through Magnetic Reluctance Coupling

International Nuclear Information System (INIS)

Pillatsch, P

2014-01-01

Energy harvesting from human motion for body worn or implanted devices faces the problem of the wearer being still, e.g. while asleep. Especially for medical devices this can become an issue if a patient is bed-bound for prolonged periods of time and the internal battery of a harvesting system is not recharged. This article introduces a mechanism for wireless energy transfer based on a previously presented energy harvesting device. The internal rotor of the energy harvester is made of mild steel and can be actuated through a magnetic reluctance coupling to an external motor. The internal piezoelectric transducer is consequently actuated and generates electricity. This paper successfully demonstrates energy transfer over a distance of 16 mm in air and an achieved power output of 85 μW at 25 Hz. The device functional volume is 1.85 cm 3 . Furthermore, it was demonstrated that increasing the driving frequency beyond 25 Hz did not yield a further increase in power output. Future research will focus on improving the reluctance coupling, e.g. by investigating the use of multiple or stronger magnets, in order to increase transmission distance

Ultrafast Mid-Infrared Intra-Excitonic Response of Individualized Single-Walled Carbon Nanotubes

International Nuclear Information System (INIS)

Wang, Jigang; Graham, Matt W.; Ma, Yingzhong; Fleming, Graham R.; Kaindl, Robert A.

2009-01-01

The quasi-1D confinement and reduced screening of photoexcited charges in single-walled carbon nanotubes (SWNTs) entails strongly-enhanced Coulomb interactions and exciton binding energies. Such amplified electron-hole (e-h) correlations have important implications for both fundamental physics and optoelectronic applications of nanotubes. The availability of 'individualized' SWNT ensembles with bright and structured luminescence has rendered specific tube chiralities experimentally accessible. In these samples, evidence for excitonic behavior was found in absorption-luminescence maps, two-photon excited luminescence, or ultrafast carrier dynamics. Here, we report ultrafast mid-infrared (mid-IR) studies of individualized SWNTs, evidencing strong photoinduced absorption around 200 meV in semiconducting tubes of (6,5) and (7,5) chiralities. This manifests the observation of quasi-1D intra-excitonic transitions between different relative-momentum states, in agreement with the binding energy and calculated oscillator strength. Our measurements further reveal a saturation of the photoinduced absorption with increasing phase-space filling of the correlated e-h pairs. The transient mid-IR response represents a new tool, unhindered by restrictions of momentum or interband dipole moment, to investigate the density and dynamics of SWNT excitons.

Tests of a prototype multiplexed fiber-optic ultra-fast FADC data acquisition system for the MAGIC telescope

International Nuclear Information System (INIS)

Bartko, H.; Goebel, F.; Mirzoyan, R.; Pimpl, W.; Teshima, M.

2005-01-01

Ground-based Atmospheric Air Cherenkov Telescopes (ACTs) are successfully used to observe very high energy (VHE) gamma rays from celestial objects. The light of the night sky (LONS) is a strong background for these telescopes. The gamma ray pulses being very short, an ultra-fast read-out of an ACT can minimize the influence of the LONS. This allows one to lower the so-called tail cuts of the shower image and the analysis energy threshold. It could also help to suppress other unwanted backgrounds. Fast 'flash' analog-to-digital converters (FADCs) with GSamples/s are available commercially; they are, however, very expensive and power consuming. Here we present a novel technique of Fiber-Optic Multiplexing which uses a single 2 GSamples/s FADC to digitize 16 read-out channels consecutively. The analog signals are delayed by using optical fibers. The multiplexed (MUX) FADC read-out reduces the cost by about 85% compared to using one ultra-fast FADC per read-out channel. Two prototype multiplexers, each digitizing data from 16 channels, were built and tested. The ultra-fast read-out system will be described and the test results will be reported. The new system will be implemented for the read-out of the 17 m diameter MAGIC telescope camera

Modeling the cooperative energy transfer dynamics of quantum cutting for solar cells

NARCIS (Netherlands)

Rabouw, Freddy T.; Meijerink, Andries

2015-01-01

Cooperative energy transfer (ET) is a quantum cutting (or downconversion) process where a luminescent center splits its excited state energy in two by simultaneous transfer to two nearby acceptor centers, thus yielding two low-energy photons for each high-energy photon absorbed. It has the potential

Quantum transfer energy in the framework of time-dependent dipole-dipole interaction

Science.gov (United States)

El-Shishtawy, Reda M.; Haddon, Robert C.; Al-Heniti, Saleh H.; Raffah, Bahaaudin M.; Berrada, K.; Abdel-Khalek, S.; Al-Hadeethi, Yas F.

2018-03-01

In this work, we examine the process of the quantum transfer of energy considering time-dependent dipole-dipole interaction in a dimer system characterized by two-level atom systems. By taking into account the effect of the acceleration and speed of the atoms in the dimer coupling, we demonstrate that the improvement of the probability for a single-excitation transfer energy extremely benefits from the incorporation of atomic motion effectiveness and the energy detuning. We explore the relevance between the population and entanglement during the time-evolution and show that this kind of nonlocal correlation may be generated during the process of the transfer of energy. Our work may provide optimal conditions to implement realistic experimental scenario in the transfer of the quantum energy.

Generation of ultrafast pulse via combined effects of stimulated

Indian Academy of Sciences (India)

A project of ultrafast pulse generation has been presented and demonstrated by utilizing the combined nonlinear effects of stimulated Raman scattering (SRS) and non-degenerate two-photon absorption (TPA) based on silicon nanophotonic chip, in which a continuous wave (CW) and an ultrafast dark pulse are ...

Inhibition of crossed-beam energy transfer induced by expansion-velocity fluctuations

Science.gov (United States)

Neuville, C.; Glize, K.; Loiseau, P.; Masson-Laborde, P.-E.; Debayle, A.; Casanova, M.; Baccou, C.; Labaune, C.; Depierreux, S.

2018-04-01

Crossed-beam energy transfer between three laser beams has been experimentally investigated in a flowing plasma. Time-evolution measurements of the amplification of a first beam by a second beam highlighted the inhibition of energy transfer by hydrodynamic modifications of the plasma in the crossing volume due to the propagation of a third beam. According to 3D simulations and an analytical model, it appears that the long-wavelength expansion-velocity fluctuations produced by the propagation of the third beam in the crossing volume are responsible for this mitigation of energy transfer. This effect could be a cause of the over-estimation of the amount of the transferred energy in indirect-drive inertial confinement fusion experiments. Besides, tuning such long-wavelength fluctuations could be a way to completely inhibit CBET at the laser entrance holes of hohlraums.

Novel Aspects of Materials Processing by Ultrafast Lasers: From Electronic to Biological and Cultural Heritage Applications

International Nuclear Information System (INIS)

Fotakis, C; Zorba, V; Stratakis, E; Athanassiou, A; Tzanetakis, P; Zergioti, I; Papagoglou, D G; Sambani, K; Filippidis, G; Farsari, M; Pouli, V; Bounos, G; Georgiou, S

2007-01-01

Materials processing by ultrafast lasers offers several distinct possibilities for micro/nano scale applications. This is due to the unique characteristics of the laser-matter interactions involved, when sub-picosecond pulses are employed. Prospects arising will be discussed in the context of surface and in bulk laser induced modifications. In particular, examples of diverse applications including the development and functionalization of laser engineered surfaces, the laser transfer of biomolecules and the functionalization of 3D structures constructed by three-photon stereolithography will be presented. Furthermore, the removal of molecular substrates by ultrafast laser ablation will be discussed with emphasis placed on assessing the photochemical changes induced in the remaining bulk material. The results indicate that in femtosecond laser processing of organic materials, besides the well acknowledged morphological advantages, a second fundamental factor responsible for its success pertains to the selective chemical effects. This is crucial for the laser cleaning of sensitive painted artworks

Modeling the efficiency of Förster resonant energy transfer from energy relay dyes in dye-sensitized solar cells

KAUST Repository

Hoke, Eric T.

2010-02-11

Förster resonant energy transfer can improve the spectral breadth, absorption and energy conversion efficiency of dye sensitized solar cells. In this design, unattached relay dyes absorb the high energy photons and transfer the excitation to sensitizing dye molecules by Förster resonant energy transfer. We use an analytic theory to calculate the excitation transfer efficiency from the relay dye to the sensitizing dye accounting for dynamic quenching and relay dye diffusion. We present calculations for pores of cylindrical and spherical geometry and examine the effects of the Förster radius, the pore size, sensitizing dye surface concentration, collisional quenching rate, and relay dye lifetime. We find that the excitation transfer efficiency can easily exceed 90% for appropriately chosen dyes and propose two different strategies for selecting dyes to achieve record power conversion efficiencies. © 2010 Optical Society of America.

RF Power Transfer, Energy Harvesting, and Power Management Strategies

Science.gov (United States)

Abouzied, Mohamed Ali Mohamed

Energy harvesting is the way to capture green energy. This can be thought of as a recycling process where energy is converted from one form (here, non-electrical) to another (here, electrical). This is done on the large energy scale as well as low energy scale. The former can enable sustainable operation of facilities, while the latter can have a significant impact on the problems of energy constrained portable applications. Different energy sources can be complementary to one another and combining multiple-source is of great importance. In particular, RF energy harvesting is a natural choice for the portable applications. There are many advantages, such as cordless operation and light-weight. Moreover, the needed infra-structure can possibly be incorporated with wearable and portable devices. RF energy harvesting is an enabling key player for Internet of Things technology. The RF energy harvesting systems consist of external antennas, LC matching networks, RF rectifiers for ac to dc conversion, and sometimes power management. Moreover, combining different energy harvesting sources is essential for robustness and sustainability. Wireless power transfer has recently been applied for battery charging of portable devices. This charging process impacts the daily experience of every human who uses electronic applications. Instead of having many types of cumbersome cords and many different standards while the users are responsible to connect periodically to ac outlets, the new approach is to have the transmitters ready in the near region and can transfer power wirelessly to the devices whenever needed. Wireless power transfer consists of a dc to ac conversion transmitter, coupled inductors between transmitter and receiver, and an ac to dc conversion receiver. Alternative far field operation is still tested for health issues. So, the focus in this study is on near field. The goals of this study are to investigate the possibilities of RF energy harvesting from various

The charge transfer structure and effective energy transfer in multiplayer assembly film

International Nuclear Information System (INIS)

Li Mingqiang; Jian Xigao

2005-01-01

Charge transfer multiplayer films have been prepared by layer-by-layer self-assembly technique. The films incorporate the rare-earth-containing polyoxometalate K 11 [Eu{PW 11 O 39 } 2 ].nH 2 O and the rich electron polyelectrolyte poly(3-viny-1-methyl-pyridine) quaternary ammonium and display a linear increase in the absorption and film thickness with the number of deposition cycles. Ultraviolet and visible absorption spectra, atomic force micrographs, small-angle X-ray reflectivity measurements, and photoluminescence spectra were used to determine the structure of films. Linear and regular multilayer growth was observed. We can observe the formation of charge transfer complex compound in multiplayer by layer-by-layer assembly method. Most importantly, the luminescence spectra show the charge transfer band in assembly films, which suggest that energy could be effectively transferred to rare earth ions in assembly multiplayer films

Energy transfers in dynamos with small magnetic Prandtl numbers

KAUST Repository

Kumar, Rohit; Verma, Mahendra K.; Samtaney, Ravi

2015-01-01

We perform numerical simulation of dynamo with magnetic Prandtl number Pm = 0.2 on 10243 grid, and compute the energy fluxes and the shell-to-shell energy transfers. These computations indicate that the magnetic energy growth takes place mainly due

Feed-forward motor control of ultrafast, ballistic movements.

Science.gov (United States)

Kagaya, K; Patek, S N

2016-02-01

To circumvent the limits of muscle, ultrafast movements achieve high power through the use of springs and latches. The time scale of these movements is too short for control through typical neuromuscular mechanisms, thus ultrafast movements are either invariant or controlled prior to movement. We tested whether mantis shrimp (Stomatopoda: Neogonodactylus bredini) vary their ultrafast smashing strikes and, if so, how this control is achieved prior to movement. We collected high-speed images of strike mechanics and electromyograms of the extensor and flexor muscles that control spring compression and latch release. During spring compression, lateral extensor and flexor units were co-activated. The strike initiated several milliseconds after the flexor units ceased, suggesting that flexor activity prevents spring release and determines the timing of strike initiation. We used linear mixed models and Akaike's information criterion to serially evaluate multiple hypotheses for control mechanisms. We found that variation in spring compression and strike angular velocity were statistically explained by spike activity of the extensor muscle. The results show that mantis shrimp can generate kinematically variable strikes and that their kinematics can be changed through adjustments to motor activity prior to the movement, thus supporting an upstream, central-nervous-system-based control of ultrafast movement. Based on these and other findings, we present a shishiodoshi model that illustrates alternative models of control in biological ballistic systems. The discovery of feed-forward control in mantis shrimp sets the stage for the assessment of targets, strategic variation in kinematics and the role of learning in ultrafast animals. © 2016. Published by The Company of Biologists Ltd.

Ultrafast Nonlinear Signal Processing in Silicon Waveguides

DEFF Research Database (Denmark)

Oxenløwe, Leif Katsuo; Mulvad, Hans Christian Hansen; Hu, Hao

2012-01-01

We describe recent demonstrations of exploiting highly nonlinear silicon waveguides for ultrafast optical signal processing. We describe wavelength conversion and serial-to-parallel conversion of 640 Gbit/s data signals and 1.28 Tbit/s demultiplexing and all-optical sampling.......We describe recent demonstrations of exploiting highly nonlinear silicon waveguides for ultrafast optical signal processing. We describe wavelength conversion and serial-to-parallel conversion of 640 Gbit/s data signals and 1.28 Tbit/s demultiplexing and all-optical sampling....

Optically nonlinear energy transfer in light-harvesting dendrimers

Science.gov (United States)

Andrews, David L.; Bradshaw, David S.

2004-08-01

Dendrimeric polymers are the subject of intense research activity geared towards their implementation in nanodevice applications such as energy harvesting systems, organic light-emitting diodes, photosensitizers, low-threshold lasers, and quantum logic elements, etc. A recent development in this area has been the construction of dendrimers specifically designed to exhibit novel forms of optical nonlinearity, exploiting the unique properties of these materials at high levels of photon flux. Starting from a thorough treatment of the underlying theory based on the principles of molecular quantum electrodynamics, it is possible to identify and characterize several optically nonlinear mechanisms for directed energy transfer and energy pooling in multichromophore dendrimers. Such mechanisms fall into two classes: first, those where two-photon absorption by individual donors is followed by transfer of the net energy to an acceptor; second, those where the excitation of two electronically distinct but neighboring donor groups is followed by a collective migration of their energy to a suitable acceptor. Each transfer process is subject to minor dissipative losses. In this paper we describe in detail the balance of factors and the constraints that determines the favored mechanism, which include the excitation statistics, structure of the energy levels, laser coherence factors, chromophore selection rules and architecture, possibilities for the formation of delocalized excitons, spectral overlap, and the overall distribution of donors and acceptors. Furthermore, it transpires that quantum interference between different mechanisms can play an important role. Thus, as the relative importance of each mechanism determines the relevant nanophotonic characteristics, the results reported here afford the means for optimizing highly efficient light-harvesting dendrimer devices.

Long-range energy transfer in self-assembled quantum dot-DNA cascades

Science.gov (United States)

Goodman, Samuel M.; Siu, Albert; Singh, Vivek; Nagpal, Prashant

2015-11-01

The size-dependent energy bandgaps of semiconductor nanocrystals or quantum dots (QDs) can be utilized in converting broadband incident radiation efficiently into electric current by cascade energy transfer (ET) between layers of different sized quantum dots, followed by charge dissociation and transport in the bottom layer. Self-assembling such cascade structures with angstrom-scale spatial precision is important for building realistic devices, and DNA-based QD self-assembly can provide an important alternative. Here we show long-range Dexter energy transfer in QD-DNA self-assembled single constructs and ensemble devices. Using photoluminescence, scanning tunneling spectroscopy, current-sensing AFM measurements in single QD-DNA cascade constructs, and temperature-dependent ensemble devices using TiO2 nanotubes, we show that Dexter energy transfer, likely mediated by the exciton-shelves formed in these QD-DNA self-assembled structures, can be used for efficient transport of energy across QD-DNA thin films.The size-dependent energy bandgaps of semiconductor nanocrystals or quantum dots (QDs) can be utilized in converting broadband incident radiation efficiently into electric current by cascade energy transfer (ET) between layers of different sized quantum dots, followed by charge dissociation and transport in the bottom layer. Self-assembling such cascade structures with angstrom-scale spatial precision is important for building realistic devices, and DNA-based QD self-assembly can provide an important alternative. Here we show long-range Dexter energy transfer in QD-DNA self-assembled single constructs and ensemble devices. Using photoluminescence, scanning tunneling spectroscopy, current-sensing AFM measurements in single QD-DNA cascade constructs, and temperature-dependent ensemble devices using TiO2 nanotubes, we show that Dexter energy transfer, likely mediated by the exciton-shelves formed in these QD-DNA self-assembled structures, can be used for efficient

Optimization and practical implementation of ultrafast 2D NMR experiments

Energy Technology Data Exchange (ETDEWEB)

Queiroz Junior, Luiz H. K., E-mail: professorkeng@gmail.com [Universidade Federal de Sao Carlos (UFSC), SP (Brazil). Departamento de Quimica; Universidade Federal de Goias (UFGO), Goiania, GO (Brazil). Inst. de Quimica; Ferreira, Antonio G. [Universidade Federal de Sao Carlos (UFSC), SP (Brazil). Departamento de Quimica; Giraudeau, Patrick [Universite de Nantes (France). CNRS, Chimie et Interdisciplinarite: Synthese, Analyse, Modelisation

2013-09-01

Ultrafast 2D NMR is a powerful methodology that allows recording of a 2D NMR spectrum in a fraction of second. However, due to the numerous non-conventional parameters involved in this methodology its implementation is no trivial task. Here, an optimized experimental protocol is carefully described to ensure efficient implementation of ultrafast NMR. The ultrafast spectra resulting from this implementation are presented based on the example of two widely used 2D NMR experiments, COSY and HSQC, obtained in 0.2 s and 41 s, respectively. (author)

Bane of Hydrogen-Bond Formation on the Photoinduced Charge-Transfer Process in Donor–Acceptor Systems

KAUST Repository

Alsam, Amani Abdu

2017-03-14

Controlling the ultrafast dynamical process of photoinduced charge transfer at donor acceptor interfaces remains a major challenge for physical chemistry and solar cell communities. The process is complicated by the involvement of other complex dynamical processes, including hydrogen bond formation, energy transfer, and solvation dynamics occurring on similar time scales. In this study, we explore the remarkable impact of hydrogen-bond formation on the interfacial charge transfer between a negatively charged electron donating anionic porphyrin and a positively charged electron accepting pi-conjugated polymer, as a model system in solvents with different polarities and capabilities for hydiogen bonding using femtosecond transient absorption spectroscopy. Unlike the conventional understanding of the key role of hydrogen bonding in promoting the charge-transfer process, our steadystate and time-resolved results reveal that the intervening hydrogen-bonding environment and, consequently, the probable longer spacing between the donor and acceptor molecules significantly hinders the charge-transfer process between them. These results show that site-specific hydrogen bonding and geometric considerations between donor and acceptor can be exploited to control both the charge-transfer dynamics and its efficiency not only at donor acceptor interfaces but also in complex biological systems.

The transfer of technologies for biomass energy utilization

International Nuclear Information System (INIS)

Schneiders, H.H.

1995-01-01

The first part of the paper presents the common perception of technology transfer as a trade relationship rather than a systematic approach to establish a complex technological capacity in a given field. It aims to correct this misperception by introducing some other ideas: (a) the need to support the people, adjust the relevant organizations and establish the capacities to provide the products and services; (b) the typical life cycles of technologies from the initial concept to the final stages of transfer and sustainable dissemination; (c) the needs and expectations of the groups targeted by the technologies for biomass energy utilization. The second part of the paper discusses one example of successful technology transfer: the use of large biomass-burning stoves for food preparation in public institutions and private restaurants in East Africa. The third part of the paper highlights two non-technological barriers to the transfer of biomass energy technologies: (a) weak market forces and business interests and a large number of State activities and projects and (b) conflicting interests of end-users, craftsmen, private and public project partners, which can threaten the success of the attempted technology transfer, even after local adaptation. Finally, suggestions are made for overcoming some of these problems. (author)

The transfer of technologies for biomass energy utilization

Energy Technology Data Exchange (ETDEWEB)

Schneiders, H H [German Agency for Technical Cooperation (GTZ), Eschborn (Germany)

1995-12-01

The first part of the paper presents the common perception of technology transfer as a trade relationship rather than a systematic approach to establish a complex technological capacity in a given field. It aims to correct this misperception by introducing some other ideas: (a) the need to support the people, adjust the relevant organizations and establish the capacities to provide the products and services; (b) the typical life cycles of technologies from the initial concept to the final stages of transfer and sustainable dissemination; (c) the needs and expectations of the groups targeted by the technologies for biomass energy utilization. The second part of the paper discusses one example of successful technology transfer: the use of large biomass-burning stoves for food preparation in public institutions and private restaurants in East Africa. The third part of the paper highlights two non-technological barriers to the transfer of biomass energy technologies: (a) weak market forces and business interests and a large number of State activities and projects and (b) conflicting interests of end-users, craftsmen, private and public project partners, which can threaten the success of the attempted technology transfer, even after local adaptation. Finally, suggestions are made for overcoming some of these problems. (author)

Delayed electron relaxation in CdTe nanorods studied by spectral analysis of the ultrafast transient absorption

International Nuclear Information System (INIS)

Kriegel, I.; Scotognella, F.; Soavi, G.; Brescia, R.; Rodríguez-Fernández, J.; Feldmann, J.; Lanzani, G.; Tassone, F.

2016-01-01

Highlights: • We study the photophysics of CdTe nanorods by ultrafast absorption spectroscopy. • We fit photobleaching and photoinduced absorption features at all time delays. • Dynamics are extracted from superpositions of bleaches (Gaussians) and derivatives. • Fast non-radiative recombination and slower hole trapping processes are extracted. • A potential approach to unveil ultrafast non-radiative recombination processes. - Abstract: In transient absorption (TA) spectra, the bleach features originating from state filling are overlapped by their energy-shifted derivatives, arising from excited state energy level shifts. This makes the direct extraction of carrier dynamics from a single-wavelength time-trace misleading. Fitting TA spectra in time, as Gaussian functions and their derivative-like shifted Gaussians, allows to individually extract the real dynamics of both photobleached transitions, and their energy shifts. In CdTe nanorods (NRs) we found a delayed heating of holes due to the release of the large excess energy in the electron relaxation process. The slow hole-trapping process is consistent with a high number of surface trap states in these model NRs. Our results show that only a correct disentanglement of bleaching and energy shift contributions provides a reliable framework to extract the underlying carrier relaxation dynamics, including trapping, non-radiative recombination, and eventually carrier multiplication.

Delayed electron relaxation in CdTe nanorods studied by spectral analysis of the ultrafast transient absorption

Energy Technology Data Exchange (ETDEWEB)

Kriegel, I., E-mail: ilka.kriegel@iit.it [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Scotognella, F. [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); CNST of IIT@POLIMI, Via Pascoli 70/3, 20133 Milano (Italy); Soavi, G. [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); Brescia, R. [Department of Nanochemistry, Istituto Italiano di Tecnologia (IIT), via Morego 30, 16163 Genova (Italy); Rodríguez-Fernández, J.; Feldmann, J. [Photonics and Optoelectronics Group, Department of Physics and CeNS, Ludwig-Maximilians-Universität München, Amalienstr. 54, 80799 Munich (Germany); Nanosystems Initiative Munich (NIM), Schellingstr. 4, 80799 Munich (Germany); Lanzani, G., E-mail: guglielmo.lanzani@iit.it [Dipartimento di Fisica, Politecnico di Milano, Piazza Leonardo da Vinci 32, 20133 Milano (Italy); CNST of IIT@POLIMI, Via Pascoli 70/3, 20133 Milano (Italy); Tassone, F. [CNST of IIT@POLIMI, Via Pascoli 70/3, 20133 Milano (Italy)

2016-06-01

Highlights: • We study the photophysics of CdTe nanorods by ultrafast absorption spectroscopy. • We fit photobleaching and photoinduced absorption features at all time delays. • Dynamics are extracted from superpositions of bleaches (Gaussians) and derivatives. • Fast non-radiative recombination and slower hole trapping processes are extracted. • A potential approach to unveil ultrafast non-radiative recombination processes. - Abstract: In transient absorption (TA) spectra, the bleach features originating from state filling are overlapped by their energy-shifted derivatives, arising from excited state energy level shifts. This makes the direct extraction of carrier dynamics from a single-wavelength time-trace misleading. Fitting TA spectra in time, as Gaussian functions and their derivative-like shifted Gaussians, allows to individually extract the real dynamics of both photobleached transitions, and their energy shifts. In CdTe nanorods (NRs) we found a delayed heating of holes due to the release of the large excess energy in the electron relaxation process. The slow hole-trapping process is consistent with a high number of surface trap states in these model NRs. Our results show that only a correct disentanglement of bleaching and energy shift contributions provides a reliable framework to extract the underlying carrier relaxation dynamics, including trapping, non-radiative recombination, and eventually carrier multiplication.

Electro-mechanical energy conversion system having a permanent magnet machine with stator, resonant transfer link and energy converter controls

Science.gov (United States)

Skeist, S. Merrill; Baker, Richard H.

2006-01-10

An electro-mechanical energy conversion system coupled between an energy source and an energy load comprising an energy converter device including a permanent magnet induction machine coupled between the energy source and the energy load to convert the energy from the energy source and to transfer the converted energy to the energy load and an energy transfer multiplexer to control the flow of power or energy through the permanent magnetic induction machine.

Quasiclassical trajectory study of the energy transfer in CO2--rare gas systems

International Nuclear Information System (INIS)

Suzukawa, H.H. Jr.; Wolfsberg, M.; Thompson, D.L.

1978-01-01

Computational methods are presented for the study of collisions between a linear, symmetric triatomic molecule and an atom by three-dimensional quasiclassical trajectory calculations. Application is made to the investigation of translational to rotational and translational to vibrational energy transfer in the systems CO 2 --Kr, CO 2 --Ar, and CO 2 --Ne. Potential-energy surfaces based on spectroscopic and molecular beam scattering data are used. In most of the calculations, the CO 2 molecule is initially in the quantum mechanical zero-point vibrational state and in a rotational state picked from a Boltzmann distribution at 300 0 K. The energy transfer processes are investigated for translational energies ranging from 0.1 to 10 eV. Translational to rotational energy transfer is found to be the major process for CO 2 --rare gas collisions at these energies. Below 1 eV there is very little translational to vibrational energy transfer. The effects of changes in the internal energy of the molecule, in the masses of the collidants, and in the potential-energy parameters are studied in an attempt to gain understanding of the energy transfer processes

All-optical temporal integration of ultrafast pulse waveforms.

Science.gov (United States)

Park, Yongwoo; Ahn, Tae-Jung; Dai, Yitang; Yao, Jianping; Azaña, José

2008-10-27

An ultrafast all-optical temporal integrator is experimentally demonstrated. The demonstrated integrator is based on a very simple and practical solution only requiring the use of a widely available all-fiber passive component, namely a reflection uniform fiber Bragg grating (FBG). This design allows overcoming the severe speed (bandwidth) limitations of the previously demonstrated photonic integrator designs. We demonstrate temporal integration of a variety of ultrafast optical waveforms, including Gaussian, odd-symmetry Hermite Gaussian, and (odd-)symmetry double pulses, with temporal features as fast as ~6-ps, which is about one order of magnitude faster than in previous photonic integration demonstrations. The developed device is potentially interesting for a multitude of applications in all-optical computing and information processing, ultrahigh-speed optical communications, ultrafast pulse (de-)coding, shaping and metrology.

Using Carbon Nanotubes for Nanometer-Scale Energy Transfer Microscopy

Science.gov (United States)

Johnston, Jessica; Shafran, Eyal; Mangum, Ben; Mu, Chun; Gerton, Jordan

2009-10-01

We investigate optical energy transfer between fluorophores and carbon nanotubes (CNTs). CNTs are grown on Si-oxide wafers by chemical vapor deposition (CVD), lifted off substrates by atomic force microscope (AFM) tips via Van der Waals forces, then shortened by electrical pulses. The tip-attached CNTs are scanned over fluorescent CdSe-ZnS quantum dots (QDs) with sub-nm precision while recording the fluorescence rate. A novel photon counting technique enables us to produce 3D maps of the QD-CNT coupling, revealing nanoscale lateral and vertical features. All CNTs tested (>50) strongly quenched the QD fluorescence, apparently independent of chirality. In some data, a delay in the recovery of QD fluorescence following CNT-QD contact was observed, suggesting possible charge transfer in this system. In the future, we will perform time-resolved studies to quantify the rate of energy and charge transfer processes and study the possible differences in fluorescence quenching and nanotube-QD energy transfer when comparing single-walled (SW) versus multi-walled (MW) CNTs, attempting to grow substrates consisting primarily of SW or MWCNTs and characterizing the structure of tip-attached CNTs using optical spectroscopy.

Ultrafast characterization of optoelectronic devices and systems

Science.gov (United States)

Zheng, Xuemei

The recent fast growth in high-speed electronics and optoelectronics has placed demanding requirements on testing tools. Electro-optic (EO) sampling is a well-established technique for characterization of high-speed electronic and optoelectronic devices and circuits. However, with the progress in device miniaturization, lower power consumption (smaller signal), and higher throughput (higher clock rate), EO sampling also needs to be updated, accordingly, towards better signal-to-noise ratio (SNR) and sensitivity, without speed sacrifice. In this thesis, a novel EO sampler with a single-crystal organic 4-dimethylamino-N-methy-4-stilbazolium tosylate (DAST) as the EO sensor is developed. The system exhibits sub-picosecond temporal resolution, sub-millivolt sensitivity, and a 10-fold improvement on SNR, compared with its LiTaO3 counterpart. The success is attributed to the very high EO coefficient, the very low dielectric constant, and the fast response, coming from the major contribution of the pi-electrons in DAST. With the advance of ultrafast laser technology, low-noise and compact femtosecond fiber lasers have come to maturation and become light-source options for ultrafast metrology systems. We have successfully integrated a femtosecond erbium-doped-fiber laser into an EO sampler, making the system compact and very reliable. The fact that EO sampling is essentially an impulse-response measurement process, requires integration of ultrashort (sub-picosecond) impulse generation network with the device under test. We have implemented a reliable lift-off and transfer technique in order to obtain epitaxial-quality freestanding low-temperature-grown GaAs (LT-GaAs) thin-film photo-switches, which can be integrated with many substrates. The photoresponse of our freestanding LT-GaAs devices was thoroughly characterized with the help of our EO sampler. As fast as 360 fs full-width-at-half-maximum (FWHM) and >1 V electrical pulses were obtained, with quantum efficiency

Active transfer of poloidal magnetic energy during plasma disruptions in J-TEXT

International Nuclear Information System (INIS)

Zhang, Ming; Zhang, Jun; Rao, Bo; Chen, Zhongyong; Li, Xiaolong; Xu, Wendi; Pan, Yuan; Yu, Kexun

2016-01-01

Highlights: • An alternative plasma disruption mitigation method by transferring partial poloidal magnetic energy out of the vacuum vessel has been presented in this paper. • This method can reduced the magnetic energy dissipated inside the vacuum vessel during disruption and mitigated the disruption damage. • This method has been experimentally verified in J-TEXT with an experiment system set up. • According to the experimental results, the magnetic energy dissipated inside the vacuum vessel during disruption can be reduced by 20% or more and the loop voltage can be reduced by 58%. - Abstract: The magnitude of the damaging effects of plasma disruptions on vacuum vessel (VV) components increases with the thermal energy and poloidal magnetic energy dissipated inside the VV. This study focuses on an alternative method, by which partial poloidal magnetic energy is transferred out of the VV. The quantity of the poloidal magnetic energy dissipated inside the VV (W_d_i_s) can be reduced with this method, and the damaging effects can be mitigated. Partial magnetic energy is transferred based on magnetic coupling by a group of energy transfer coils (ETCs) that are coupled with the plasma current. This method, which is called magnetic energy transfer (MET), has been experimentally verified in J-TEXT. W_d_i_s can be reduced by approximately 20%, and the loop voltage can be reduced by 58%. MET is established as a novel, promising, and effective plasma disruption mitigation method.

PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

Science.gov (United States)

Kono, Junichiro

2013-02-01

Journal of Physics: Condensed Matter staff for their help, patience and professionalism. Since this is a fast-moving field, there is absolutely no way of presenting definitive answers to all open questions, but we hope that this special section will provide an overview of the current state of knowledge regarding this topic. Furthermore, we hope that the exciting science and technology described in this section will attract and inspire other researchers and students working in related fields to enter into the study of ultrafast and nonlinear optical phenomena in carbon-based nanostructures. Ultrafast and nonlinear optics in carbon nanomaterials contents Ultrafast and nonlinear optics in carbon nanomaterialsJunichiro Kono The impact of pump fluence on carrier relaxation dynamics in optically excited grapheneT Winzer and E Malic Time-resolved spectroscopy on epitaxial graphene in the infrared spectral range: relaxation dynamics and saturation behaviorS Winnerl, F Göttfert, M Mittendorff, H Schneider, M Helm, T Winzer, E Malic, A Knorr, M Orlita, M Potemski, M Sprinkle, C Berger and W A de Heer Nonlinear optics of graphene in a strong magnetic fieldXianghan Yao and Alexey Belyanin Theory of coherent phonons in carbon nanotubes and graphene nanoribbonsG D Sanders, A R T Nugraha, K Sato, J-H Kim3, J Kono3, R Saito and C J Stanton Non-perturbative effects of laser illumination on the electrical properties of graphene nanoribbons Hernán L Calvo, Pablo M Perez-Piskunow, Horacio M Pastawski, Stephan Roche and Luis E F Foa Torres Transient absorption microscopy studies of energy relaxation in graphene oxide thin film Sean Murphy and Libai Huang Femtosecond dynamics of exciton localization: self-trapping from the small to the large polaron limit F X Morrissey, J G Mance, A D Van Pelt and S L Dexheimer

Novel DNA sequence detection method based on fluorescence energy transfer

International Nuclear Information System (INIS)

Kobayashi, S.; Tamiya, E.; Karube, I.

1987-01-01

Recently the detection of specific DNA sequence, DNA analysis, has been becoming more important for diagnosis of viral genomes causing infections disease and human sequences related to inherited disorders. These methods typically involve electrophoresis, the immobilization of DNA on a solid support, hybridization to a complementary probe, the detection using labeled with /sup 32/P or nonisotopically with a biotin-avidin-enzyme system, and so on. These techniques are highly effective, but they are very time-consuming and expensive. A principle of fluorescene energy transfer is that the light energy from an excited donor (fluorophore) is transferred to an acceptor (fluorophore), if the acceptor exists in the vicinity of the donor and the excitation spectrum of donor overlaps the emission spectrum of acceptor. In this study, the fluorescence energy transfer was applied to the detection of specific DNA sequence using the hybridization method. The analyte, single-stranded DNA labeled with the donor fluorophore is hybridized to a probe DNA labeled with the acceptor. Because of the complementary DNA duplex formation, two fluorophores became to be closed to each other, and the fluorescence energy transfer was occurred

Ultra-fast electron capture by electrosterically-stabilized gold nanoparticles.

Science.gov (United States)

Ghandi, Khashayar; Findlater, Alexander D; Mahimwalla, Zahid; MacNeil, Connor S; Awoonor-Williams, Ernest; Zahariev, Federico; Gordon, Mark S

2015-07-21

Ultra-fast pre-solvated electron capture has been observed for aqueous solutions of room-temperature ionic liquid (RTIL) surface-stabilized gold nanoparticles (AuNPs; ∼9 nm). The extraordinarily large inverse temperature dependent rate constants (k(e)∼ 5 × 10(14) M(-1) s(-1)) measured for the capture of electrons in solution suggest electron capture by the AuNP surface that is on the timescale of, and therefore in competition with, electron solvation and electron-cation recombination reactions. The observed electron transfer rates challenge the conventional notion that radiation induced biological damage would be enhanced in the presence of AuNPs. On the contrary, AuNPs stabilized by non-covalently bonded ligands demonstrate the potential to quench radiation-induced electrons, indicating potential applications in fields ranging from radiation therapy to heterogeneous catalysis.

Ultrafast electron diffraction studies of optically excited thin bismuth films

International Nuclear Information System (INIS)

Rajkovic, Ivan

2008-01-01

This thesis contains work on the design and the realization of an experimental setup capable of providing sub-picosecond electron pulses for ultrafast electron diffraction experiments, and performing the study of ultrafast dynamics in bismuth after optical excitation using this setup. (orig.)

Ultrafast electron diffraction studies of optically excited thin bismuth films

Energy Technology Data Exchange (ETDEWEB)

Rajkovic, Ivan

2008-10-21

This thesis contains work on the design and the realization of an experimental setup capable of providing sub-picosecond electron pulses for ultrafast electron diffraction experiments, and performing the study of ultrafast dynamics in bismuth after optical excitation using this setup. (orig.)

Femtosecond spectroscopy of bacterial photosynthesis--towards an understanding of the most important energy conversion process on earth

International Nuclear Information System (INIS)

Zinth, W.; Hamm, P.; Arlt, T.; Wachtveitl, J.

1996-01-01

Reaction centers of bacterial photosynthesis are ideal systems to study photosynthetic energy conversion. Femtosecond spectroscopy has delivered extensive information on the molecular mechanisms of the primary electron transfer. The data show, that primary electron transfer is an ultrafast stepwise reaction, where the electron is transferred via closely spaced pigments with reaction times as fast as 0.9 ps and 3.5 ps. Experiments on mutated and modified reaction centers allow to determine the energetics of the various intermediates in the reaction center. Recently, femtosecond experiments with light pulses in the mid infrared have shown, that an additional fast process occurs on the 200 fs timescale in the initially excited special pair. Only afterwards the well established electron transfer reactions take place. This fast process may be of importance for the optimization of the primary reaction

Nuclear energy technology transfer: the security barriers

International Nuclear Information System (INIS)

Rinne, R.L.

1975-08-01

The problems presented by security considerations to the transfer of nuclear energy technology are examined. In the case of fusion, the national security barrier associated with the laser and E-beam approaches is discussed; for fission, the international security requirements, due to the possibility of the theft or diversion of special nuclear materials or sabotage of nuclear facilities, are highlighted. The paper outlines the nuclear fuel cycle and terrorist threat, examples of security barriers, and the current approaches to transferring technology. (auth)

Static and Ultrafast Transient Photophysics of Mono- and Dual-Branched Triarylamines

International Nuclear Information System (INIS)

Feng-Ming, Li; Wen-Ke, Feng; Shu-Feng, Wang; Qi-Huang, Gong; Fan-Shun, Meng; He, Tian

2010-01-01

Mono- and dual-branched molecules, {4-[2-(4-benzothiazol-2-yl-phenyl)-vinyl]-phenyl}-(4-methoxy-phenyl) -phenyl-amine (BS1) and bis-{4-[2-(4-benzothiazol-2-yl-phenyl)-vinyl]-phenyl}-(4-methoxy-phenyl) -phenyl-amine (BS2), are investigated with one- and two-photon static spectroscopy, and the femtosecond fluorescence up-conversion technique. The molecules show branch-based fluorescence emission at low quantum yield. Ultrafast non-radiative decay on a picosecond time scale is found and is attributed to intramolecular charge-transfer bridged by the central triphenylamine. The two-photon absorption cross-sections of BS1 and BS2 are 19.1 and 19.4 GM, respectively. (cross-disciplinary physics and related areas of science and technology)

Long range energy transfer in graphene hybrid structures

International Nuclear Information System (INIS)

Gonçalves, Hugo; Bernardo, César; Moura, Cacilda; Belsley, Michael; Schellenberg, Peter; Ferreira, R A S; André, P S; Stauber, Tobias

2016-01-01

In this work we quantify the distance dependence for the extraction of energy from excited chromophores by a single layer graphene flake over a large separation range. To this end hybrid structures were prepared, consisting of a thin (2 nm) layer of a polymer matrix doped with a well chosen strongly fluorescent organic molecule, followed by an un-doped spacer layer of well-defined thicknesses made of the same polymer material and an underlying single layer of pristine, undoped graphene. The coupling strength is assessed through the variation of the fluorescence decay kinetics as a function of distance between the graphene and the excited chromophore molecules. Non-radiative energy transfer to the graphene was observed at distances of up to 60 nm; a range much greater than typical energy transfer distances observed in molecular systems. (paper)

Ultrafast magnon generation in an Fe film on Cu(100).

Science.gov (United States)

Schmidt, A B; Pickel, M; Donath, M; Buczek, P; Ernst, A; Zhukov, V P; Echenique, P M; Sandratskii, L M; Chulkov, E V; Weinelt, M

2010-11-05

We report on a combined experimental and theoretical study of the spin-dependent relaxation processes in the electron system of an iron film on Cu(100). Spin-, time-, energy- and angle-resolved two-photon photoemission shows a strong characteristic dependence of the lifetime of photoexcited electrons on their spin and energy. Ab initio calculations as well as a many-body treatment corroborate that the observed properties are determined by relaxation processes involving magnon emission. Thereby we demonstrate that magnon emission by hot electrons occurs on the femtosecond time scale and thus provides a significant source of ultrafast spin-flip processes. Furthermore, engineering of the magnon spectrum paves the way for tuning the dynamic properties of magnetic materials.

Progress in ultrafast intense laser science XI

CERN Document Server

Yamanouchi, Kaoru; Martin, Philippe

2014-01-01

The PUILS series delivers up-to-date reviews of progress in Ultrafast Intense Laser Science, a newly emerging interdisciplinary research field spanning atomic and molecular physics, molecular science and optical science, which has been stimulated by the recent developments in ultrafast laser technologies. Each volume compiles peer-reviewed articles authored by researchers at the forefront of each their own subfields of UILS. Every chapter opens with an overview of the topics to be discussed, so that researchers unfamiliar to the subfield, as well as graduate students, can grasp the importance

Progress in Ultrafast Intense Laser Science II

CERN Document Server

Yamanouchi, Kaoru; Agostini, Pierre; Ferrante, Gaetano

2007-01-01

This book series addresses a newly emerging interdisciplinary research field, Ultrafast Intense Laser Science, spanning atomic and molecular physics, molecular science, and optical science. Its progress is being stimulated by the recent development of ultrafast laser technologies. Highlights of this second volume include Coulomb explosion and fragmentation of molecules, control of chemical dynamics, high-order harmonic generation, propagation and filamentation, and laser-plasma interaction. All chapters are authored by foremost experts in their fields and the texts are written at a level accessible to newcomers and graduate students, each chapter beginning with an introductory overview.

Heat transfer coefficient of cryotop during freezing.

Science.gov (United States)

Li, W J; Zhou, X L; Wang, H S; Liu, B L; Dai, J J

2013-01-01

Cryotop is an efficient vitrification method for cryopreservation of oocytes. It has been widely used owing to its simple operation and high freezing rate. Recently, the heat transfer performance of cryotop was studied by numerical simulation in several studies. However, the range of heat transfer coefficient in the simulation is uncertain. In this study, the heat transfer coefficient for cryotop during freezing process was analyzed. The cooling rates of 40 percent ethylene glycol (EG) droplet in cryotop during freezing were measured by ultra-fast measurement system and calculated by numerical simulation at different value of heat transfer coefficient. Compared with the results obtained by two methods, the range of the heat transfer coefficient necessary for the numerical simulation of cryotop was determined, which is between 9000 W/(m(2)·K) and 10000 W/(m (2)·K).

Mega-electron-volt ultrafast electron diffraction at SLAC National Accelerator Laboratory

Energy Technology Data Exchange (ETDEWEB)

Weathersby, S. P.; Brown, G.; Chase, T. F.; Coffee, R.; Corbett, J.; Eichner, J. P.; Frisch, J. C.; Fry, A. R.; Gühr, M.; Hartmann, N.; Hast, C.; Hettel, R.; Jobe, R. K.; Jongewaard, E. N.; Lewandowski, J. R.; Li, R. K., E-mail: lrk@slac.stanford.edu; Lindenberg, A. M.; Makasyuk, I.; May, J. E.; McCormick, D. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); and others

2015-07-15

Ultrafast electron probes are powerful tools, complementary to x-ray free-electron lasers, used to study structural dynamics in material, chemical, and biological sciences. High brightness, relativistic electron beams with femtosecond pulse duration can resolve details of the dynamic processes on atomic time and length scales. SLAC National Accelerator Laboratory recently launched the Ultrafast Electron Diffraction (UED) and microscopy Initiative aiming at developing the next generation ultrafast electron scattering instruments. As the first stage of the Initiative, a mega-electron-volt (MeV) UED system has been constructed and commissioned to serve ultrafast science experiments and instrumentation development. The system operates at 120-Hz repetition rate with outstanding performance. In this paper, we report on the SLAC MeV UED system and its performance, including the reciprocal space resolution, temporal resolution, and machine stability.

Bane of Hydrogen-Bond Formation on the Photoinduced Charge-Transfer Process in Donor–Acceptor Systems

KAUST Repository

Alsam, Amani Abdu; Adhikari, Aniruddha; Parida, Manas R.; Aly, Shawkat Mohammede; Bakr, Osman; Mohammed, Omar F.

2017-01-01

Controlling the ultrafast dynamical process of photoinduced charge transfer at donor acceptor interfaces remains a major challenge for physical chemistry and solar cell communities. The process is complicated by the involvement of other complex

Ultrafast electron microscopy in materials science, biology, and chemistry

International Nuclear Information System (INIS)

King, Wayne E.; Campbell, Geoffrey H.; Frank, Alan; Reed, Bryan; Schmerge, John F.; Siwick, Bradley J.; Stuart, Brent C.; Weber, Peter M.

2005-01-01

The use of pump-probe experiments to study complex transient events has been an area of significant interest in materials science, biology, and chemistry. While the emphasis has been on laser pump with laser probe and laser pump with x-ray probe experiments, there is a significant and growing interest in using electrons as probes. Early experiments used electrons for gas-phase diffraction of photostimulated chemical reactions. More recently, scientists are beginning to explore phenomena in the solid state such as phase transformations, twinning, solid-state chemical reactions, radiation damage, and shock propagation. This review focuses on the emerging area of ultrafast electron microscopy (UEM), which comprises ultrafast electron diffraction (UED) and dynamic transmission electron microscopy (DTEM). The topics that are treated include the following: (1) The physics of electrons as an ultrafast probe. This encompasses the propagation dynamics of the electrons (space-charge effect, Child's law, Boersch effect) and extends to relativistic effects. (2) The anatomy of UED and DTEM instruments. This includes discussions of the photoactivated electron gun (also known as photogun or photoelectron gun) at conventional energies (60-200 keV) and extends to MeV beams generated by rf guns. Another critical aspect of the systems is the electron detector. Charge-coupled device cameras and microchannel-plate-based cameras are compared and contrasted. The effect of various physical phenomena on detective quantum efficiency is discussed. (3) Practical aspects of operation. This includes determination of time zero, measurement of pulse-length, and strategies for pulse compression. (4) Current and potential applications in materials science, biology, and chemistry. UEM has the potential to make a significant impact in future science and technology. Understanding of reaction pathways of complex transient phenomena in materials science, biology, and chemistry will provide fundamental

Design of a variable-phase contactless energy transfer platform using air-cored planar inductor technology

NARCIS (Netherlands)

Sonntag, C.L.W.

2010-01-01

Contactless Energy Transfer (CET) describes the process in which electrical energy is transferred among two or more galvanically isolated electrical circuits or devices by means of magnetic induction (magnetic energy). The potential applications can range from the transfer of energy between low

Energy transfer in scattering by rotating potentials

Indian Academy of Sciences (India)

R. Narasimhan (Krishtel eMaging) 1461 1996 Oct 15 13:05:22

Quantum mechanical scattering theory is studied for time-dependent. Schrödinger ... the energy transferred to a particle by collision with a rotating blade. Keywords. ..... terms of the unitary group for some time-independent generator. This will ...

Vectorial photoinduced energy transfer between boron-dipyrromethene (Bodipy) chromophores across a fluorene bridge.

Science.gov (United States)

Puntoriero, Fausto; Nastasi, Francesco; Campagna, Sebastiano; Bura, Thomas; Ziessel, Raymond

2010-08-02

A series of novel multichromophoric, luminescent compounds has been prepared, and their absorption spectra, luminescence properties (both at 77 K in rigid matrix and at 298 K in fluid solution), and photoinduced intercomponent energy-transfer processes have been studied. The series contains two new multichromophoric systems 1 and 2, each one containing two different boron-dipyrromethene (Bodipy) subunits and one bridging fluorene species, and two fluorene-Bodipy bichromophoric species, 6 and 7. Three monochromophoric compounds, 3, 4, and 5, used as precursors in the synthetic process, were also fully characterized. The absorption spectra of the multichromophoric compounds are roughly the summation of the absorption spectra of their individual components, thus demonstrating the supramolecular nature of the assemblies. Luminescence studies show that quantitative energy transfer occurs in 6 and 7 from the fluorene chromophore to the Bodipy dyes. Luminescence studies, complemented by transient-absorption spectroscopy studies, also indicate that efficient inter-Bodipy energy transfer across the rigid fluorene spacer takes place in 1 and 2, with rate constants, evaluated by several experimental methods, between 2.0 and 7.0 x 10(9) s(-1). Such an inter-Bodipy energy transfer appears to be governed by the Förster mechanism. By taking advantage of the presence of various protonable sites in the substituents of the lower-energy Bodipy subunit of 1 and 2, the effect of protonation on the energy-transfer rates has also been investigated. The results suggest that control of energy-transfer rate and efficiency of inter-Bodipy energy transfer in this type of systems can be achieved by an external, reversible input.

Ultrafast exciton decay in PbS quantum dots through simultaneous electron and hole recombination with a surface-localized ion pair

Energy Technology Data Exchange (ETDEWEB)

Edme, Kedy; Bettis Homan, Stephanie; Nepomnyashchii, Alexander B.; Weiss, Emily A., E-mail: e-weiss@northwestern.edu

2016-06-01

Highlights: • We synthesize complexes of PbS quantum dots (QDs) and tetracyanoquinodimethane (TCNQ). Each PbS QD spontaneously reduces up to 17 TCNQ molecules. • The photoluminescence of the PbS QDs is quenched in the presence of the reduced TCNQ species through ultrafast non-radiative, simultaneous decay of the electron and hole. • We assign this decay to a four-carrier, concerted charge recombination mechanism with the surface localized sulfur–TCNQ{sup x−} ion pair. - Abstract: This paper describes the ultrafast decay of the band-edge exciton in PbS quantum dots (QDs) through simultaneous recombination of the excitonic hole and electron with the surface localized ion pair formed upon adsorption of tetracyanoquinodimethane (TCNQ). Each PbS QD (R = 1.8 nm) spontaneously reduces up to 17 TCNQ molecules upon adsorption of the TCNQ molecule to a sulfur on the QD surface. The photoluminescence of the PbS QDs is quenched in the presence of the reduced TCNQ species through ultrafast (⩽15-ps) non-radiative decay of the exciton; the rate constant for the decay process increases approximately linearly with the number of adsorbed, reduced TCNQ molecules. Near-infrared and mid-infrared transient absorption show that this decay occurs through simultaneous transfer of the excitonic electron and hole, and is assigned to a four-carrier, concerted charge recombination mechanism based on the observations that (i) the PL of the QDs recovers when spontaneously reduced TCNQ{sup 1−} desorbs from the QD surface upon addition of salt, and (ii) the PL of the QDs is preserved when another spontaneous oxidant, ferrocinium, which cannot participate in charge transfer in its reduced state, is substituted for TCNQ.

Efficient light emission from inorganic and organic semiconductor hybrid structures by energy-level tuning.

Science.gov (United States)

Schlesinger, R; Bianchi, F; Blumstengel, S; Christodoulou, C; Ovsyannikov, R; Kobin, B; Moudgil, K; Barlow, S; Hecht, S; Marder, S R; Henneberger, F; Koch, N

2015-04-15

The fundamental limits of inorganic semiconductors for light emitting applications, such as holographic displays, biomedical imaging and ultrafast data processing and communication, might be overcome by hybridization with their organic counterparts, which feature enhanced frequency response and colour range. Innovative hybrid inorganic/organic structures exploit efficient electrical injection and high excitation density of inorganic semiconductors and subsequent energy transfer to the organic semiconductor, provided that the radiative emission yield is high. An inherent obstacle to that end is the unfavourable energy level offset at hybrid inorganic/organic structures, which rather facilitates charge transfer that quenches light emission. Here, we introduce a technologically relevant method to optimize the hybrid structure's energy levels, here comprising ZnO and a tailored ladder-type oligophenylene. The ZnO work function is substantially lowered with an organometallic donor monolayer, aligning the frontier levels of the inorganic and organic semiconductors. This increases the hybrid structure's radiative emission yield sevenfold, validating the relevance of our approach.

Efficient light emission from inorganic and organic semiconductor hybrid structures by energy-level tuning

Science.gov (United States)

Schlesinger, R.; Bianchi, F.; Blumstengel, S.; Christodoulou, C.; Ovsyannikov, R.; Kobin, B.; Moudgil, K.; Barlow, S.; Hecht, S.; Marder, S.R.; Henneberger, F.; Koch, N.

2015-01-01

The fundamental limits of inorganic semiconductors for light emitting applications, such as holographic displays, biomedical imaging and ultrafast data processing and communication, might be overcome by hybridization with their organic counterparts, which feature enhanced frequency response and colour range. Innovative hybrid inorganic/organic structures exploit efficient electrical injection and high excitation density of inorganic semiconductors and subsequent energy transfer to the organic semiconductor, provided that the radiative emission yield is high. An inherent obstacle to that end is the unfavourable energy level offset at hybrid inorganic/organic structures, which rather facilitates charge transfer that quenches light emission. Here, we introduce a technologically relevant method to optimize the hybrid structure's energy levels, here comprising ZnO and a tailored ladder-type oligophenylene. The ZnO work function is substantially lowered with an organometallic donor monolayer, aligning the frontier levels of the inorganic and organic semiconductors. This increases the hybrid structure's radiative emission yield sevenfold, validating the relevance of our approach. PMID:25872919

Power Loss Analysis and Comparison of Segmented and Unsegmented Energy Coupling Coils for Wireless Energy Transfer.

Science.gov (United States)

Tang, Sai Chun; McDannold, Nathan J

2015-03-01

This paper investigated the power losses of unsegmented and segmented energy coupling coils for wireless energy transfer. Four 30-cm energy coupling coils with different winding separations, conductor cross-sectional areas, and number of turns were developed. The four coils were tested in both unsegmented and segmented configurations. The winding conduction and intrawinding dielectric losses of the coils were evaluated individually based on a well-established lumped circuit model. We found that the intrawinding dielectric loss can be as much as seven times higher than the winding conduction loss at 6.78 MHz when the unsegmented coil is tightly wound. The dielectric loss of an unsegmented coil can be reduced by increasing the winding separation or reducing the number of turns, but the power transfer capability is reduced because of the reduced magnetomotive force. Coil segmentation using resonant capacitors has recently been proposed to significantly reduce the operating voltage of a coil to a safe level in wireless energy transfer for medical implants. Here, we found that it can naturally eliminate the dielectric loss. The coil segmentation method and the power loss analysis used in this paper could be applied to the transmitting, receiving, and resonant coils in two- and four-coil energy transfer systems.

Wireless energy transfer: Dielectric lens antennas for beam shaping in wireless power-transfer applications

Science.gov (United States)

Gonçalves, Ricardo; Carvalho, Nuno B.; Pinho, Pedro

2017-02-01

In the current contest of wireless systems, the last frontier remains the cut of the power cord. In that sense, the interest over wireless energy transfer technologies in the past years has grown exponentially. However, there are still many challenges to be overcome in order to enable wireless energy transfer full potential. One of the focus in the development of such systems is the design of very-high-gain, highly efficient, antennas that can compensate for the propagation loss of radio signals over the air. In this paper, we explore the design and manufacturing process of dielectric lenses, fabricated using a professional-grade desktop 3D printer. Lens antennas are used in order to increase beam efficiency and therefore maximize the efficiency of a wireless power-transfer system operating at microwave frequencies in the Ku band. Measurements of two fabricated prototypes showcase a large directivity, as predicted with simulations. xml:lang="fr"

Ultrafast dynamics of ligand and substrate interaction in endothelial nitric oxide synthase under Soret excitation.

Science.gov (United States)

Hung, Chih-Chang; Yabushita, Atsushi; Kobayashi, Takayoshi; Chen, Pei-Feng; Liang, Keng S

2016-01-01

Ultrafast transient absorption spectroscopy of endothelial NOS oxygenase domain (eNOS-oxy) was performed to study dynamics of ligand or substrate interaction under Soret band excitation. Photo-excitation dissociates imidazole ligand in 4ps. The eNOS-oxy without additive is partially bound with water molecule, thus its photoexcited dynamics also shows ligand dissociation in <800fs. Then it followed by vibrational cooling coupled with charge transfer in 4.8ps, and recombination of ligand to distal side of heme in 12ps. Copyright © 2016 Elsevier B.V. All rights reserved.

Higher order energy transfer. Quantum electrodynamical calculations and graphical representation

International Nuclear Information System (INIS)

Jenkins, R.D.

2000-01-01

In Chapter 1, a novel method of calculating quantum electrodynamic amplitudes is formulated using combinatorial theory. This technique is used throughout instead of conventional time-ordered methods. A variety of hyperspaces are discussed to highlight isomorphism between a number of A generalisation of Pascal's triangle is shown to be beneficial in determining the form of hyperspace graphs. Chapter 2 describes laser assisted resonance energy transfer (LARET), a higher order perturbative contribution to the well-known process resonance energy transfer, accommodating an off resonance auxiliary laser field to stimulate the migration. Interest focuses on energy exchanges between two uncorrelated molecular species, as in a system where molecules are randomly oriented. Both phase-weighted and standard isotropic averaging are required for the calculations. Results are discussed in terms of a laser intensity-dependent mechanism. Identifying the applied field regime where LARET should prove experimentally significant, transfer rate increases of up to 30% are predicted. General results for three-center energy transfer are elucidated in chapter 3. Cooperative and accretive mechanistic pathways are identified with theory formulated to elicit their role in a variety of energy transfer phenomena and their relative dominance. In multichromophoric the interplay of such factors is analysed with regard to molecular architectures. The alignments and magnitudes of donor and acceptor transition moments and polarisabilities prove to have profound effects on achievable pooling efficiency for linear configurations. Also optimum configurations are offered. In ionic lattices, although both mechanisms play significant roles in pooling and cutting processes, only the accretive is responsible for sensitisation. The local, microscopic level results are used to gauge the lattice response, encompassing concentration and structural effects. (author)

Resonance Energy Transfer in Hybrid Devices in the Presence of a Surface

DEFF Research Database (Denmark)

Kopylov, Oleksii; Huck, Alexander; Kadkhodazadeh, Shima

2014-01-01

to approximately 10 nm was observed. By comparing the carrier dynamics of the quantum wells and the nanocrystals, we found that nonradiative recombination via surface states, generated during dry etching of the wafer, counteracts the nonradiative energy-transfer process to the nanocrystals and therefore decreases......We have studied room-temperature, nonradiative resonant energy transfer from InGaN/GaN quantum wells to CdSe/ZnS nanocrystals separated by aluminum oxide layers of different thicknesses. Nonradiative energy transfer from the quantum wells to the nanocrystals at separation distances of up...

State-Resolved Metal Nanoparticle Dynamics Viewed through the Combined Lenses of Ultrafast and Magneto-optical Spectroscopies.

Science.gov (United States)

Zhao, Tian; Herbert, Patrick J; Zheng, Hongjun; Knappenberger, Kenneth L

2018-05-08

Electronic carrier dynamics play pivotal roles in the functional properties of nanomaterials. For colloidal metals, the mechanisms and influences of these dynamics are structure dependent. The coherent carrier dynamics of collective plasmon modes for nanoparticles (approximately 2 nm and larger) determine optical amplification factors that are important to applied spectroscopy techniques. In the nanocluster domain (sub-2 nm), carrier coupling to vibrational modes affects photoluminescence yields. The performance of photocatalytic materials featuring both nanoparticles and nanoclusters also depends on the relaxation dynamics of nonequilibrium charge carriers. The challenges for developing comprehensive descriptions of carrier dynamics spanning both domains are multifold. Plasmon coherences are short-lived, persisting for only tens of femtoseconds. Nanoclusters exhibit discrete carrier dynamics that can persist for microseconds in some cases. On this time scale, many state-dependent processes, including vibrational relaxation, charge transfer, and spin conversion, affect carrier dynamics in ways that are nonscalable but, rather, structure specific. Hence, state-resolved spectroscopy methods are needed for understanding carrier dynamics in the nanocluster domain. Based on these considerations, a detailed understanding of structure-dependent carrier dynamics across length scales requires an appropriate combination of spectroscopic methods. Plasmon mode-specific dynamics can be obtained through ultrafast correlated light and electron microscopy (UCLEM), which pairs interferometric nonlinear optical (INLO) with electron imaging methods. INLO yields nanostructure spectral resonance responses, which capture the system's homogeneous line width and coherence dynamics. State-resolved nanocluster dynamics can be obtained by pairing ultrafast with magnetic-optical spectroscopy methods. In particular, variable-temperature variable-field (VTVH) spectroscopies allow quantification

Probing Ultrafast Electron Dynamics at Surfaces Using Soft X-Ray Transient Reflectivity Spectroscopy

Science.gov (United States)

Baker, L. Robert; Husek, Jakub; Biswas, Somnath; Cirri, Anthony

The ability to probe electron dynamics with surface sensitivity on the ultrafast time scale is critical for understanding processes such as charge separation, injection, and surface trapping that mediate efficiency in catalytic and energy conversion materials. Toward this goal, we have developed a high harmonic generation (HHG) light source for femtosecond soft x-ray reflectivity. Using this light source we investigated the ultrafast carrier dynamics at the surface of single crystalline α-Fe2O3, polycrystalline α-Fe2O3, and the mixed metal oxide, CuFeO2. We have recently demonstrated that CuFeO2 in particular is a selective catalyst for photo-electrochemical CO2 reduction to acetate; however, the role of electronic structure and charge carrier dynamics in mediating catalytic selectivity has not been well understood. Soft x-ray reflectivity measurements probe the M2,3, edges of the 3d transition metals, which provide oxidation and spin state resolution with element specificity. In addition to chemical state specificity, these measurements are also surface sensitive, and by independently simulating the contributions of the real and imaginary components of the complex refractive index, we can differentiate between surface and sub-surface contributions to the excited state spectrum. Accordingly, this work demonstrates the ability to probe ultrafast carrier dynamics in catalytic materials with element and chemical state specificity and with surface sensitivity.

Exciton dynamics in an energy up-converting solid state system based on diphenylanthracene doped with platinum octaethylporphyrin

Energy Technology Data Exchange (ETDEWEB)

Karpicz, R., E-mail: renata.karpicz@ftmc.lt [Center for Physical Sciences and Technology, Savanoriu Ave. 231, LT-02300 Vilnius (Lithuania); Puzinas, S.; Gulbinas, V. [Center for Physical Sciences and Technology, Savanoriu Ave. 231, LT-02300 Vilnius (Lithuania); Vakhnin, A. [Institute of Physics, National Academy of Sciences of Ukraine, 03028 Kyiv (Ukraine); Kadashchuk, A. [Institute of Physics, National Academy of Sciences of Ukraine, 03028 Kyiv (Ukraine); IMEC, Kapeldreef 75, B-3001 Heverlee-Leuven (Belgium); Rand, B.P. [IMEC, Kapeldreef 75, B-3001 Heverlee-Leuven (Belgium); Department of Electrical Engineering and the Andlinger Center for Energy and the Environment, Princeton University, Princeton, NJ 08544 (United States)

2014-01-31

Highlights: • We study exciton dynamics by ultrafast spectroscopies in DPA:PtOEP host–guest films. • Aggregation of PtOEP affects considerably the triplet energy transfer to DPA host. • No significant triplet loss due to TTA occurs within PtOEP aggregates. • Triplet energy transfer from PtOEP to DPA is slow and thermally activated process. • The ISC time in PtOEP is shorter than 100 fs. - Abstract: Photophysics of composite solid films based on 9,10-diphenylanthracene (DPA) doped with Pt(II)octaethylporphyrin (PtOEP) has been investigated by means of transient absorption and luminescence spectroscopy. The DPA:PtOEP host:guest system is a benchmark for incoherent energy up-conversion via triplet fusion in solution and we focus here on photophysical processes of this system in solid films. The triplet energy transfer from PtOEP to DPA takes place during tens of ns, featuring a thermally activated behavior. This implies that, before being transferred to the host, triplets migrate within PtOEP aggregates, defining a rate limiting step for the overall energy transfer to DPA. In contrast to other porphyrin-based sensitizers, no significant triplet–triplet annihilation was found to happen during triplet migration within PtOEP aggregates, implying that such a triplet loss mechanism does not universally apply to porphyrin-based organometallic complexes.

Carrier dynamics in graphene. Ultrafast many-particle phenomena

Energy Technology Data Exchange (ETDEWEB)

Malic, E.; Brem, S.; Jago, R. [Department of Physics, Chalmers University of Technology, Goeteborg (Sweden); Winzer, T.; Wendler, F.; Knorr, A. [Institut fuer Theoretische Physik, Technische Universitaet Berlin (Germany); Mittendorff, M.; Koenig-Otto, J.C.; Schneider, H.; Helm, M.; Winnerl, S. [Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany); Ploetzing, T.; Neumaier, D. [Advanced Microelectronic Center Aachen, AMO GmbH, Aachen (Germany)

2017-11-15

Graphene is an ideal material to study fundamental Coulomb- and phonon-induced carrier scattering processes. Its remarkable gapless and linear band structure opens up new carrier relaxation channels. In particular, Auger scattering bridging the valence and the conduction band changes the number of charge carriers and gives rise to a significant carrier multiplication - an ultrafast many-particle phenomenon that is promising for the design of highly efficient photodetectors. Furthermore, the vanishing density of states at the Dirac point combined with ultrafast phonon-induced intraband scattering results in an accumulation of carriers and a population inversion suggesting the design of graphene-based terahertz lasers. Here, we review our work on the ultrafast carrier dynamics in graphene and Landau-quantized graphene is presented providing a microscopic view on the appearance of carrier multiplication and population inversion. (copyright 2017 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

Ultrafast electric phase control of a single exciton qubit

Science.gov (United States)

Widhalm, Alex; Mukherjee, Amlan; Krehs, Sebastian; Sharma, Nandlal; Kölling, Peter; Thiede, Andreas; Reuter, Dirk; Förstner, Jens; Zrenner, Artur

2018-03-01

We report on the coherent phase manipulation of quantum dot excitons by electric means. For our experiments, we use a low capacitance single quantum dot photodiode which is electrically controlled by a custom designed SiGe:C BiCMOS chip. The phase manipulation is performed and quantified in a Ramsey experiment, where ultrafast transient detuning of the exciton energy is performed synchronous to double pulse π/2 ps laser excitation. We are able to demonstrate electrically controlled phase manipulations with magnitudes up to 3π within 100 ps which is below the dephasing time of the quantum dot exciton.

WE-B-210-02: The Advent of Ultrafast Imaging in Biomedical Ultrasound

International Nuclear Information System (INIS)

Tanter, M.

2015-01-01

In the last fifteen years, the introduction of plane or diverging wave transmissions rather than line by line scanning focused beams has broken the conventional barriers of ultrasound imaging. By using such large field of view transmissions, the frame rate reaches the theoretical limit of physics dictated by the ultrasound speed and an ultrasonic map can be provided typically in tens of micro-seconds (several thousands of frames per second). Interestingly, this leap in frame rate is not only a technological breakthrough but it permits the advent of completely new ultrasound imaging modes, including shear wave elastography, electromechanical wave imaging, ultrafast doppler, ultrafast contrast imaging, and even functional ultrasound imaging of brain activity (fUltrasound) introducing Ultrasound as an emerging full-fledged neuroimaging modality. At ultrafast frame rates, it becomes possible to track in real time the transient vibrations – known as shear waves – propagating through organs. Such “human body seismology” provides quantitative maps of local tissue stiffness whose added value for diagnosis has been recently demonstrated in many fields of radiology (breast, prostate and liver cancer, cardiovascular imaging, …). Today, Supersonic Imagine company is commercializing the first clinical ultrafast ultrasound scanner, Aixplorer with real time Shear Wave Elastography. This is the first example of an ultrafast Ultrasound approach surpassing the research phase and now widely spread in the clinical medical ultrasound community with an installed base of more than 1000 Aixplorer systems in 54 countries worldwide. For blood flow imaging, ultrafast Doppler permits high-precision characterization of complex vascular and cardiac flows. It also gives ultrasound the ability to detect very subtle blood flow in very small vessels. In the brain, such ultrasensitive Doppler paves the way for fUltrasound (functional ultrasound imaging) of brain activity with unprecedented

WE-B-210-02: The Advent of Ultrafast Imaging in Biomedical Ultrasound

Energy Technology Data Exchange (ETDEWEB)

Tanter, M. [Laboratoire Ondes et Acoustique (France)

2015-06-15

In the last fifteen years, the introduction of plane or diverging wave transmissions rather than line by line scanning focused beams has broken the conventional barriers of ultrasound imaging. By using such large field of view transmissions, the frame rate reaches the theoretical limit of physics dictated by the ultrasound speed and an ultrasonic map can be provided typically in tens of micro-seconds (several thousands of frames per second). Interestingly, this leap in frame rate is not only a technological breakthrough but it permits the advent of completely new ultrasound imaging modes, including shear wave elastography, electromechanical wave imaging, ultrafast doppler, ultrafast contrast imaging, and even functional ultrasound imaging of brain activity (fUltrasound) introducing Ultrasound as an emerging full-fledged neuroimaging modality. At ultrafast frame rates, it becomes possible to track in real time the transient vibrations – known as shear waves – propagating through organs. Such “human body seismology” provides quantitative maps of local tissue stiffness whose added value for diagnosis has been recently demonstrated in many fields of radiology (breast, prostate and liver cancer, cardiovascular imaging, …). Today, Supersonic Imagine company is commercializing the first clinical ultrafast ultrasound scanner, Aixplorer with real time Shear Wave Elastography. This is the first example of an ultrafast Ultrasound approach surpassing the research phase and now widely spread in the clinical medical ultrasound community with an installed base of more than 1000 Aixplorer systems in 54 countries worldwide. For blood flow imaging, ultrafast Doppler permits high-precision characterization of complex vascular and cardiac flows. It also gives ultrasound the ability to detect very subtle blood flow in very small vessels. In the brain, such ultrasensitive Doppler paves the way for fUltrasound (functional ultrasound imaging) of brain activity with unprecedented

Coherent combination of ultrafast fiber amplifiers

International Nuclear Information System (INIS)

Hanna, Marc; Guichard, Florent; Druon, Frédéric; Georges, Patrick; Zaouter, Yoann; Papadopoulos, Dimitris N

2016-01-01

We review recent progress in coherent combining of femtosecond pulses amplified in optical fibers as a way to scale the peak and average power of ultrafast sources. Different methods of achieving coherent pulse addition in space (beam combining) and time (divided pulse amplification) domains are described. These architectures can be widely classified into active methods, where the relative phases between pulses are subject to a servomechanism, and passive methods, where phase matching is inherent to the geometry. Other experiments that combine pulses with different spectral contents, pulses that have been nonlinearly broadened or successive pulses from a mode-locked laser oscillator, are then presented. All these techniques allow access to unprecedented parameter range for fiber ultrafast sources. (topical review)

Ultrafast single-molecule photonics: Excited state dynamics in coherently coupled complexes

International Nuclear Information System (INIS)

Hernando, Jordi; Hoogenboom, Jacob; Dijk, Erik van; Garcia-Parajo, Maria; Hulst, Niek F. van

2008-01-01

We present a single-molecule study on femtosecond dynamics in multichromophoric systems, combining fs pump-probe, emission-spectra and fluorescence-lifetime analysis. The ultrafast fs approach gives direct information on the initial exciton dynamics after excitation. The lifetime data show superradiance, a direct measure for the extent of the coherent coupling and static disorder. The spectra finally reveal the role of exciton-phonon coupling. At the single-molecule level a wide range of exciton delocalization lengths and energy redistribution times is revealed

Ultrafast single-molecule photonics: Excited state dynamics in coherently coupled complexes

Energy Technology Data Exchange (ETDEWEB)

Hernando, Jordi [Dept. de Quimica, Universitat Autonoma Barcelona, 08193 Cerdanyola del Valles (Spain); Hoogenboom, Jacob [ICFO-Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels, Barcelona (Spain); Dijk, Erik van [Applied Optics Group, MESA Institute for Nanotechnology, University of Twente, 7500AE Enschede (Netherlands); Garcia-Parajo, Maria [IBEC-Institute of BioEngineering of Catalunya, 08028 Barcelona (Spain); ICREA-Institucio Catalana de Recerca i Estudis Avancats, 08015 Barcelona (Spain); Hulst, Niek F. van [ICFO-Institut de Ciencies Fotoniques, Mediterranean Technology Park, 08860 Castelldefels, Barcelona (Spain) and ICREA-Institucio Catalana de Recerca i Estudis Avancats, 08015 Barcelona (Spain)], E-mail: Niek.vanHulst@ICFO.es

2008-05-15

We present a single-molecule study on femtosecond dynamics in multichromophoric systems, combining fs pump-probe, emission-spectra and fluorescence-lifetime analysis. The ultrafast fs approach gives direct information on the initial exciton dynamics after excitation. The lifetime data show superradiance, a direct measure for the extent of the coherent coupling and static disorder. The spectra finally reveal the role of exciton-phonon coupling. At the single-molecule level a wide range of exciton delocalization lengths and energy redistribution times is revealed.

Tracking of the nuclear wavepacket motion in cyanine photoisomerization by ultrafast pump-dump-probe spectroscopy.

Science.gov (United States)

Wei, Zhengrong; Nakamura, Takumi; Takeuchi, Satoshi; Tahara, Tahei

2011-06-01

Understanding ultrafast reactions, which proceed on a time scale of nuclear motions, requires a quantitative characterization of the structural dynamics. To track such structural changes with time, we studied a nuclear wavepacket motion in photoisomerization of a prototype cyanine dye, 1,1'-diethyl-4,4'-cyanine, by ultrafast pump-dump-probe measurements in solution. The temporal evolution of wavepacket motion was examined by monitoring the efficiency of stimulated emission dumping, which was obtained from the recovery of a ground-state bleaching signal. The dump efficiency versus pump-dump delay exhibited a finite rise time, and it became longer (97 fs → 330 fs → 390 fs) as the dump pulse was tuned to longer wavelengths (690 nm → 950 nm → 1200 nm). This result demonstrates a continuous migration of the leading edge of the wavepacket on the excited-state potential from the Franck-Condon region toward the potential minimum. A slowly decaying feature of the dump efficiency indicated a considerable broadening of the wavepacket over a wide range of the potential, which results in the spread of a population distribution on the flat S(1) potential energy surface. The rapid migration as well as broadening of the wavepacket manifests a continuous nature of the structural dynamics and provides an intuitive visualization of this ultrafast reaction. We also discussed experimental strategies to evaluate reliable dump efficiencies separately from other ultrafast processes and showed a high capability and possibility of the pump-dump-probe method for spectroscopic investigation of unexplored potential regions such as conical intersections. © 2011 American Chemical Society

Ultrafast optical signal processing using semiconductor quantum dot amplifiers

DEFF Research Database (Denmark)

Berg, Tommy Winther; Mørk, Jesper

2002-01-01

The linear and nonlinear properties of quantum dot amplifiers are discussed on the basis of an extensive theoretical model. These devices show great potential for linear amplification as well as ultrafast signal processing.......The linear and nonlinear properties of quantum dot amplifiers are discussed on the basis of an extensive theoretical model. These devices show great potential for linear amplification as well as ultrafast signal processing....

Risk transfer via energy-savings insurance

International Nuclear Information System (INIS)

Mills, Evan

2003-01-01

Among the key barriers to investment in energy efficiency are uncertainties about attaining projected energy savings and potential disputes over stipulated savings. The fields of energy management and risk management are thus intertwined. While many technical methods have emerged to manage performance risks (e.g. building diagnostics and commissioning), financial methods are less developed in the energy management arena than in other segments of the economy. Energy-savings insurance (ESI) - formal insurance of predicted energy savings - transfers and spreads both types of risk over a larger pool of energy efficiency projects and reduces barriers to market entry of smaller energy service firms who lack sufficiently strong balance sheets to self-insure the savings. ESI encourages those implementing energy-saving projects to go beyond standard measures and thereby achieve more significant levels of energy savings. Insurance providers are proponents of improved savings measurement and verification techniques, as well as maintenance, thereby contributing to national energy-saving objectives. If properly applied, ESI can potentially reduce the net cost of energy-saving projects by reducing the interest rates charged by lenders, and by increasing the level of savings through quality control. Governmental agencies have been pioneers in the use of ESI and could continue to play a role

Energy relaxation and transfer in excitonic trimer

International Nuclear Information System (INIS)

Herman, Pavel; Barvik, Ivan; Urbanec, Martin

2004-01-01

Two models describing exciton relaxation and transfer (the Redfield model in the secular approximation and Capek's model) are compared for a simple example - a symmetric trimer coupled to a phonon bath. Energy transfer within the trimer occurs via resonance interactions and coupling between the trimer and the bath occurs via modulation of the monomer energies by phonons. Two initial conditions are adopted: (1) one of higher eigenstates of the trimer is initially occupied and (2) one local site of the trimer is initially occupied. The diagonal exciton density matrix elements in the representation of eigenstates are found to be the same for both models, but this is not so for the off-diagonal density matrix elements. Only if the off-diagonal density matrix elements vanish initially (initial condition (1)), they then vanish at arbitrary times in both models. If the initial excitation is local, the off-diagonal matrix elements essentially differ

Solar wind energy transfer through the magnetopause of an open magnetosphere

International Nuclear Information System (INIS)

Lee, L.C.; Roederer, J.G.

1982-01-01

An expression for the total power P/sub T/ transferred from the solar wind to an ''open'' magnetopause with a nonzero normal component of the magnetic field, which is identified as a rotational discontinuity. The total power P/sub T/ consists of (1) the power P/sub EM/ representing the electromagnetic energy transfer and (2) the power P/sub KE/ representing the rate of kinetic energy carried by particles penetrating into the magnetosphere. It is found that P/sub EM/approx. =V/sub SW/ B/sub SW/psi, P/sub KE/approx. =(1/2 M/sub A/-1) P/sub EM/ and P/sub T/approx. =1/2M/sub A/P/sub EM/, where V/sub SW/, B/sub SW/, and M/sub A/ are the velocity, magnetic field, and the Alfven--Mach number in the solar wind, respectively, and Psi is the open magnetic flux in the magnetosphere. The Alfven--Mach number of flow at the magnetopause determines the nature of the local energy transfer; the power per unit area transferred from the solar wind to the magnetosphere consists mainly of kinetic energy. The electromagnetic energy rate P/sub EM/ controls the near-earth magnetospheric activity, whereas the kinetic energy rate P/sub KE/(approx. =3--4 P/sub EM/) should dominate the dynamics of the distant magnetotail

Photoinduced charge and energy transfer in dye-doped conjugated polymers

International Nuclear Information System (INIS)

Veldman, Dirk; Bastiaansen, Jolanda J.A.M.; Langeveld-Voss, Bea M.W.; Sweelssen, Joergen; Koetse, Marc M.; Meskers, Stefan C.J.; Janssen, Rene A.J.

2006-01-01

Conjugated polymer-molecular dye blends of MDMO-PPV (poly[2-methoxy-5-(3',7'-dimethyloctyloxy)-1,4-phenylenevinylene]) and PF1CVTP (poly[9,9-dioctylfluorene-2,7-diyl-alt-2,5-bis(2-thienyl-1-cyanovinyl) -1-(3',7= '-dimethyloctyloxy)-4-methoxybenzene-5'',5''-diyl]) with three dipyrrometheneboron difluoride (bodipy) dyes were studied by (time-resolved) fluorescence and photoinduced absorption spectroscopy to determine quantitatively the relation between the electronic HOMO and LUMO levels and the occurrence of energy or charge transfer after optical excitation. We find that for MDMO-PPV photoinduced charge transfer to the dyes occurs, while photoexcitation of PF1CVTP exclusively results in energy transfer. The differences can be rationalized by assuming that the energy of the charge separated state is 0.33-0.45 eV higher than the energy determined from oxidation and reduction potentials of donor and acceptor, respectively. This provides an important design rule to identify appropriate materials for polymer solar cells that can have a high open-circuit voltage

Resonant electronic excitation energy transfer by Dexter mechanism in the quantum dot system

Science.gov (United States)

Samosvat, D. M.; Chikalova-Luzina, O. P.; Vyatkin, V. M.; Zegrya, G. G.

2016-11-01

In present work the energy transfer between quantum dots by the exchange (Dexter) mechanism is analysed. The interdot Coulomb interaction is taken into consideration. It is assumed that the quantum dot-donor and the quantum dot-acceptor are made from the same compound A3B5 and embedded in the matrix of other material creating potential barriers for electron and holes. The dependences of the energy transfer rate on the quantum-dot system parameters are found using the Kane model that provides the most adequate description spectra of semiconductors A3B5. Numerical calculations show that the rate of the energy transfer by Dexter mechanism is comparable to the rate of the energy transfer by electrostatic mechanism at the distances approaching to the contact ones.

Femtosecond stimulated Raman evidence for charge-transfer character in pentacene singlet fission.

Science.gov (United States)

Hart, Stephanie M; Silva, W Ruchira; Frontiera, Renee R

2018-02-07

Singlet fission is a spin-allowed process in which an excited singlet state evolves into two triplet states. We use femtosecond stimulated Raman spectroscopy, an ultrafast vibrational technique, to follow the molecular structural evolution during singlet fission in order to determine the mechanism of this process. In crystalline pentacene, we observe the formation of an intermediate characterized by pairs of excited state peaks that are red- and blue-shifted relative to the ground state features. We hypothesize that these features arise from the formation of cationic and anionic species due to partial transfer of electron density from one pentacene molecule to a neighboring molecule. These observations provide experimental evidence for the role of states with significant charge-transfer character which facilitate the singlet fission process in pentacene. Our work both provides new insight into the singlet fission mechanism in pentacene and demonstrates the utility of structurally-sensitive time-resolved spectroscopic techniques in monitoring ultrafast processes.

Photosynthetic Energy Transfer at the Quantum/Classical Border.

Science.gov (United States)

Keren, Nir; Paltiel, Yossi

2018-06-01

Quantum mechanics diverges from the classical description of our world when very small scales or very fast processes are involved. Unlike classical mechanics, quantum effects cannot be easily related to our everyday experience and are often counterintuitive to us. Nevertheless, the dimensions and time scales of the photosynthetic energy transfer processes puts them close to the quantum/classical border, bringing them into the range of measurable quantum effects. Here we review recent advances in the field and suggest that photosynthetic processes can take advantage of the sensitivity of quantum effects to the environmental 'noise' as means of tuning exciton energy transfer efficiency. If true, this design principle could be a base for 'nontrivial' coherent wave property nano-devices. Copyright © 2018 Elsevier Ltd. All rights reserved.

Toward understanding as photosynthetic biosignatures: light harvesting and energy transfer calculation

Science.gov (United States)

Komatsu, Y.; Umemura, M.; Shoji, M.; Shiraishi, K.; Kayanuma, M.; Yabana, K.

2014-03-01

Among several proposed biosignatures, red edge is a direct evidence of photosynthetic life if it is detected (Kiang et al 2007). Red edge is a sharp change in reflectance spectra of vegetation in NIR region (about 700-750 nm). The sign of red edge is observed by Earthshine or remote sensing (Wolstencroft & Raven 2002, Woolf et al 2002). But, why around 700-750 nm? The photosynthetic organisms on Earth have evolved to optimize the sunlight condition. However, if we consider about photosynthetic organism on extrasolar planets, they should have developed to utilize the spectra of its principal star. Thus, it is not strange even if it shows different vegetation spectra. In this study, we focused on the light absorption mechanism of photosynthetic organisms on Earth and investigated the fundamental properties of the light harvesting mechanisms, which is the first stage for the light absorption. Light harvesting complexes contain photosynthetic pigments like chlorophylls. Effective light absorption and the energy transfer are accomplished by the electronic excitations of collective photosynthetic pigments. In order to investigate this mechanism, we constructed an energy transfer model by using a dipole-dipole approximation for the interactions between electronic excitations. Transition moments and transition energies of each pigment are calculated at the time-dependent density functional theory (TDDFT) level (Marques & Gross 2004). Quantum dynamics simulation for the excitation energy transfer was calculated by the Liouvelle's equation. We adopted the model to purple bacteria, which has been studied experimentally and known to absorb lower energy. It is meaningful to focus on the mechanism of this bacteria, since in the future mission, M planets will become a important target. We calculated the oscillator strengths in one light harvesting complex and confirmed the validity by comparing to the experimental data. This complex is made of an inner and an outer ring. The

Infrared laser driven double proton transfer. An optimal control theory study

Science.gov (United States)

Abdel-Latif, Mahmoud K.; Kühn, Oliver

2010-02-01

Laser control of ultrafast double proton transfer is investigated for a two-dimensional model system describing stepwise and concerted transfer pathways. The pulse design has been done by employing optimal control theory in combination with the multiconfiguration time-dependent Hartree wave packet propagation. The obtained laser fields correspond to multiple pump-dump pulse sequences. Special emphasis is paid to the relative importance of stepwise and concerted transfer pathways for the driven wave packet and its dependence on the parameters of the model Hamiltonian as well as on the propagation time. While stepwise transfer is dominating in all cases considered, for high barrier systems concerted transfer proceeding via tunneling can make a contribution.

Ultrafast vibrations of gold nanorings

DEFF Research Database (Denmark)

Kelf, T; Tanaka, Y; Matsuda, O

2011-01-01

We investigate the vibrational modes of gold nanorings on a silica substrate with an ultrafast optical technique. By comparison with numerical simulations, we identify several resonances in the gigahertz range associated with axially symmetric deformations of the nanoring and substrate. We...

Ultrafast Spectroscopy of Semiconductor Devices

DEFF Research Database (Denmark)

Borri, Paola; Langbein, Wolfgang; Hvam, Jørn Marcher

1999-01-01

In this work we present an experimental technique for investigating ultrafast carrier dynamics in semiconductor optical amplifiers at room temperature. These dynamics, influenced by carrier heating, spectral hole-burning and two-photon absorption, are very important for device applications in inf...

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

Reduced Charge Transfer Exciton Recombination in Organic Semiconductor Heterojunctions by Molecular Doping

Science.gov (United States)

Deschler, Felix; da Como, Enrico; Limmer, Thomas; Tautz, Raphael; Godde, Tillmann; Bayer, Manfred; von Hauff, Elizabeth; Yilmaz, Seyfullah; Allard, Sybille; Scherf, Ullrich; Feldmann, Jochen

2011-09-01

We investigate the effect of molecular doping on the recombination of electrons and holes localized at conjugated-polymer-fullerene interfaces. We demonstrate that a low concentration of p-type dopant molecules (<4% weight) reduces the interfacial recombination via charge transfer excitons and results in a favored formation of separated carriers. This is observed by the ultrafast quenching of photoluminescence from charge transfer excitons and the increase in photoinduced polaron density by ˜70%. The results are consistent with a reduced formation of emissive charge transfer excitons, induced by state filling of tail states.

Exciton and Hole-Transfer Dynamics in Polymer: Fullerene Blends

Directory of Open Access Journals (Sweden)

van Loosdrecht P. H. M.

2013-03-01

Full Text Available Ultrafast hole transfer dynamics from fullerene derivative to polymer in bulk heterojunction blends are studied with visible-pump - IR-probe spectroscopy. The hole transfer process is found to occur in 50/300 fs next to the interface, while a longer 15-ps time is attributed to exciton diffusion towards interface in PC71BM domains. High polaron generation efficiency in P3HT blends indicates excellent intercalation between the polymer and the fullerene even at highest PC71BM concentration thereby yielding a valuable information on the blend morphology.

Energy transfer and clustering of photosynthetic light-harvesting complexes in reconstituted lipid membranes

International Nuclear Information System (INIS)

Dewa, Takehisa; Sumino, Ayumi; Watanabe, Natsuko; Noji, Tomoyasu; Nango, Mamoru

2013-01-01

Highlights: ► Photosynthetic light-harvesting complexes were reconstituted into lipid membranes. ► Energy transfers between light-harvesting complexes were examined. ► Atomic force microscopy indicated cluster formation of light-harvesting complexes. ► Efficient energy transfer was observed for the clustered complexes in the membranes. - Abstract: In purple photosynthetic bacteria, light-harvesting complex 2 (LH2) and light harvesting/reaction centre core complex (LH1-RC) play the key roles of capturing and transferring light energy and subsequent charge separation. These photosynthetic apparatuses form a supramolecular assembly; however, how the assembly influences the efficiency of energy conversion is not yet clear. We addressed this issue by evaluating the energy transfer in reconstituted photosynthetic protein complexes LH2 and LH1-RC and studying the structures and the membrane environment of the LH2/LH1-RC assemblies, which had been embedded into various lipid bilayers. Thus, LH2 and LH1-RC from Rhodopseudomonas palustris 2.1.6 were reconstituted in phosphatidylglycerol (PG), phosphatidylcholine (PC), and phosphatidylethanolamine (PE)/PG/cardiolipin (CL). Efficient energy transfer from LH2 to LH1-RC was observed in the PC and PE/PG/CL membranes. Atomic force microscopy revealed that LH2 and LH1-RC were heterogeneously distributed to form clusters in the PC and PE/PG/CL membranes. The results indicated that the phospholipid species influenced the cluster formation of LH2 and LH1-RC as well as the energy transfer efficiency

Energy transfer and clustering of photosynthetic light-harvesting complexes in reconstituted lipid membranes

Energy Technology Data Exchange (ETDEWEB)

Dewa, Takehisa, E-mail: takedewa@nitech.ac.jp [Department of Frontier Materials, Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); Japan Science and Technology, PRESTO, 4-1-8 Honcho Kawaguchi, Saitama 332-0012 (Japan); Sumino, Ayumi; Watanabe, Natsuko; Noji, Tomoyasu [Department of Frontier Materials, Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan); Nango, Mamoru, E-mail: nango@nitech.ac.jp [Department of Frontier Materials, Graduate School of Engineering, Nagoya Institute of Technology, Gokiso-cho, Showa-ku, Nagoya 466-8555 (Japan)

2013-06-20

Highlights: ► Photosynthetic light-harvesting complexes were reconstituted into lipid membranes. ► Energy transfers between light-harvesting complexes were examined. ► Atomic force microscopy indicated cluster formation of light-harvesting complexes. ► Efficient energy transfer was observed for the clustered complexes in the membranes. - Abstract: In purple photosynthetic bacteria, light-harvesting complex 2 (LH2) and light harvesting/reaction centre core complex (LH1-RC) play the key roles of capturing and transferring light energy and subsequent charge separation. These photosynthetic apparatuses form a supramolecular assembly; however, how the assembly influences the efficiency of energy conversion is not yet clear. We addressed this issue by evaluating the energy transfer in reconstituted photosynthetic protein complexes LH2 and LH1-RC and studying the structures and the membrane environment of the LH2/LH1-RC assemblies, which had been embedded into various lipid bilayers. Thus, LH2 and LH1-RC from Rhodopseudomonas palustris 2.1.6 were reconstituted in phosphatidylglycerol (PG), phosphatidylcholine (PC), and phosphatidylethanolamine (PE)/PG/cardiolipin (CL). Efficient energy transfer from LH2 to LH1-RC was observed in the PC and PE/PG/CL membranes. Atomic force microscopy revealed that LH2 and LH1-RC were heterogeneously distributed to form clusters in the PC and PE/PG/CL membranes. The results indicated that the phospholipid species influenced the cluster formation of LH2 and LH1-RC as well as the energy transfer efficiency.

Ultrafast Gap Dynamics and Electronic Interactions in a Photoexcited Cuprate Superconductor

Directory of Open Access Journals (Sweden)

S. Parham

2017-10-01

Full Text Available We perform time- and angle-resolved photoemission spectroscopy (trARPES on optimally doped Bi_{2}Sr_{2}CaCu_{2}O_{8+δ} (BSCCO-2212 using sufficient energy resolution (9 meV to resolve the k-dependent near-nodal gap structure on time scales where the concept of an electronic pseudotemperature is a useful quantity, i.e., after electronic thermalization has occurred. We study the ultrafast evolution of this gap structure, uncovering a very rich landscape of decay rates as a function of angle, temperature, and energy. We explicitly focus on the quasiparticle states at the gap edge as well as on the spectral weight inside the gap that “fills” the gap—understood as an interaction, or self-energy effect—and we also make high resolution measurements of the nodal states, enabling a direct and accurate measurement of the electronic temperature (or pseudotemperature of the electrons in the system. Rather than the standard method of interpreting these results using individual quasiparticle scattering rates that vary significantly as a function of angle, temperature, and energy, we show that the entire landscape of relaxations can be understood by modeling the system as following a nonequilibrium, electronic pseudotemperature that controls all electrons in the zone. Furthermore, this model has zero free parameters, as we obtain the crucial information of the SC gap Δ and the gap-filling strength Γ_{TDoS} by connecting to static ARPES measurements. The quantitative and qualitative agreement between data and model suggests that the critical parameters and interactions of the system, including the pairing interactions, follow parametrically from the electronic pseudotemperature. We expect that this concept will be relevant for understanding the ultrafast response of a great variety of electronic materials, even though the electronic pseudotemperature may not be directly measurable.

Efficient weakly-radiative wireless energy transfer: An EIT-like approach

International Nuclear Information System (INIS)

Hamam, Rafif E.; Karalis, Aristeidis; Joannopoulos, J.D.; Soljacic, Marin

2009-01-01

Inspired by a quantum interference phenomenon known in the atomic physics community as electromagnetically induced transparency (EIT), we propose an efficient weakly radiative wireless energy transfer scheme between two identical classical resonant objects, strongly coupled to an intermediate classical resonant object of substantially different properties, but with the same resonance frequency. The transfer mechanism essentially makes use of the adiabatic evolution of an instantaneous (so called 'dark') eigenstate of the coupled 3-object system. Our analysis is based on temporal coupled mode theory (CMT), and is general enough to be valid for various possible sorts of coupling, including the resonant inductive coupling on which witricity-type wireless energy transfer is based. We show that in certain parameter regimes of interest, this scheme can be more efficient, and/or less radiative than other, more conventional approaches. A concrete example of wireless energy transfer between capacitively-loaded metallic loops is illustrated at the beginning, as a motivation for the more general case. We also explore the performance of the currently proposed EIT-like scheme, in terms of improving efficiency and reducing radiation, as the relevant parameters of the system are varied.

Ultrafast demagnetisation dependence on film thickness: A TDDFT calculation

Science.gov (United States)

Singh, N.; Sharma, S.

2018-04-01

Ferromagnetic materials when subjected to intense laser pulses leads to reduction of their magnetisation on an ultrafast scale. Here, we perform an ab-initio calculation to study the behavior of ultrafast demagnetisation as a function of film thickness for Nickel as compared to the bulk of the material. In thin films surface formation results in amplification of demagnetisation with the percentage of demagnetisation depending upon the film thickness.

On the relation between Marcus theory and ultrafast spectroscopy of solvation kinetics

Science.gov (United States)

Roy, Santanu; Galib, Mirza; Schenter, Gregory K.; Mundy, Christopher J.

2018-01-01

The phenomena of solvent exchange control the process of solvating ions, protons, and charged molecules. Building upon our extension of Marcus' philosophy of electron transfer, we provide a new perspective of ultrafast solvent exchange mechanism around ions measurable by two-dimensional infrared (2DIR) spectroscopy. In this theory, solvent rearrangement drives an ion-bound water to an activated state of higher coordination number, triggering ion-water separation that leads to the solvent-bound state of the water molecule. This ion-bound to solvent-bound transition rate for a BF4--water system is computed using ab initio molecular dynamics and Marcus theory, and is found to be in excellent agreement with the 2DIR measurement.

Can nanophotonics control the Förster resonance energy transfer efficiency?

DEFF Research Database (Denmark)

Blum, C.; Zijlstra, N.; Lagendijk, A.

2013-01-01

from photovoltaics and lighting, to probing molecular distances and interactions.It is an intriguing open question whether the FRET rate γFRET and the energy transfer efficiency ηFRET can also be controlled by the nanoscale optical environment, characterized by the local density of optical states (LDOS...... precisely-defined, isolated, and efficient donor-acceptor pairs. The FRET pairs are dye molecules that covalently bound to the opposite ends of a 15 basepair long double-stranded with a precisely defined distance of 6.8 nm. Control over the LDOS is realized by positioning the FRET systems at well...... of the energy donor by the LDOS, the energy transfer efficiency can be enhanced or reduced. If a donor with unit quantum efficiency is placed in a 3D photonic bandgap, the energy transfer efficiency will approach 100 %, independent of the acceptor, and of the distances and orientations between the FRET partners....

Ultra-Fast Hadronic Calorimetry

Energy Technology Data Exchange (ETDEWEB)

Denisov, Dmitri [Fermilab; Lukić, Strahinja [VINCA Inst. Nucl. Sci., Belgrade; Mokhov, Nikolai [Fermilab; Striganov, Sergei [Fermilab; Ujić, Predrag [VINCA Inst. Nucl. Sci., Belgrade

2017-12-18

Calorimeters for particle physics experiments with integration time of a few ns will substantially improve the capability of the experiment to resolve event pileup and to reject backgrounds. In this paper time development of hadronic showers induced by 30 and 60 GeV positive pions and 120 GeV protons is studied using Monte Carlo simulation and beam tests with a prototype of a sampling steel-scintillator hadronic calorimeter. In the beam tests, scintillator signals induced by hadronic showers in steel are sampled with a period of 0.2 ns and precisely time-aligned in order to study the average signal waveform at various locations w.r.t. the beam particle impact. Simulations of the same setup are performed using the MARS15 code. Both simulation and test beam results suggest that energy deposition in steel calorimeters develop over a time shorter than 3 ns providing opportunity for ultra-fast calorimetry. Simulation results for an "ideal" calorimeter consisting exclusively of bulk tungsten or copper are presented to establish the lower limit of the signal integration window.

Ultrafast magnetodynamics with free-electron lasers

Science.gov (United States)

Malvestuto, Marco; Ciprian, Roberta; Caretta, Antonio; Casarin, Barbara; Parmigiani, Fulvio

2018-02-01

The study of ultrafast magnetodynamics has entered a new era thanks to the groundbreaking technological advances in free-electron laser (FEL) light sources. The advent of these light sources has made possible unprecedented experimental schemes for time-resolved x-ray magneto-optic spectroscopies, which are now paving the road for exploring the ultimate limits of out-of-equilibrium magnetic phenomena. In particular, these studies will provide insights into elementary mechanisms governing spin and orbital dynamics, therefore contributing to the development of ultrafast devices for relevant magnetic technologies. This topical review focuses on recent advancement in the study of non-equilibrium magnetic phenomena from the perspective of time-resolved extreme ultra violet (EUV) and soft x-ray spectroscopies at FELs with highlights of some important experimental results.

Femtochemistry and femtobiology ultrafast dynamics in molecular science

CERN Document Server

Douhal, Abderrazzak

2002-01-01

This book contains important contributions from top international scientists on the-state-of-the-art of femtochemistry and femtobiology at the beginning of the new millennium. It consists of reviews and papers on ultrafast dynamics in molecular science.The coverage of topics highlights several important features of molecular science from the viewpoint of structure (space domain) and dynamics (time domain). First of all, the book presents the latest developments, such as experimental techniques for understanding ultrafast processes in gas, condensed and complex systems, including biological mol

Photoinduced energy and electron transfer in rubrene-benzoquinone and rubrene-porphyrin systems

KAUST Repository

Khan, Jafar Iqbal

2014-11-01

Excited-state electron and energy transfer from singlet excited rubrene (Ru) to benzoquinone (BQ) and tetra-(4-aminophenyl) porphyrin (TAPP) were investigated by steady-state absorption and emission, time-resolved transient absorption, and femtosecond (fs)-nanosecond (ns) fluorescence spectroscopy. The low reduction potential of BQ provides the high probability of electron transfer from the excited Ru to BQ. Steady-state and time-resolved results confirm such an excited electron transfer scenario. On the other hand, strong spectral overlap between the emission of Ru and absorption of TAPP suggests that energy transfer is a possible deactivation pathway of the Ru excited state.

Resonant electronic excitation energy transfer by Dexter mechanism in the quantum dot system

International Nuclear Information System (INIS)

Samosvat, D M; Chikalova-Luzina, O P; Zegrya, G G; Vyatkin, V M

2016-01-01

In present work the energy transfer between quantum dots by the exchange (Dexter) mechanism is analysed. The interdot Coulomb interaction is taken into consideration. It is assumed that the quantum dot-donor and the quantum dot-acceptor are made from the same compound A3B5 and embedded in the matrix of other material creating potential barriers for electron and holes. The dependences of the energy transfer rate on the quantum-dot system parameters are found using the Kane model that provides the most adequate description spectra of semiconductors A3B5. Numerical calculations show that the rate of the energy transfer by Dexter mechanism is comparable to the rate of the energy transfer by electrostatic mechanism at the distances approaching to the contact ones. (paper)

Ultrafast spectroscopy of biological photoreceptors

NARCIS (Netherlands)

Kennis, J.T.M.; Groot, M.L.

2007-01-01

We review recent new insights on reaction dynamics of photoreceptors proteins gained from ultrafast spectroscopy. In Blue Light sensing Using FAD (BLUF) domains, a hydrogen-bond rearrangement around the flavin chromophore proceeds through a radical-pair mechanism, by which light-induced electron and

Ultrafast vibrations of gold nanorings

DEFF Research Database (Denmark)

Kelf, T; Tanaka, Y; Matsuda, O

2011-01-01

We investigate the vibrational modes of gold nanorings on a silica substrate with an ultrafast optical technique. By comparison with numerical simulations, we identify several resonances in the gigahertz range associated with axially symmetric deformations of the nanoring and substrate. We elucid...

Ultrafast surface-enhanced Raman spectroscopy.

Science.gov (United States)

Keller, Emily L; Brandt, Nathaniel C; Cassabaum, Alyssa A; Frontiera, Renee R

2015-08-07

Ultrafast surface-enhanced Raman spectroscopy (SERS) with pico- and femtosecond time resolution has the ability to elucidate the mechanisms by which plasmons mediate chemical reactions. Here we review three important technological advances in these new methodologies, and discuss their prospects for applications in areas including plasmon-induced chemistry and sensing at very low limits of detection. Surface enhancement, arising from plasmonic materials, has been successfully incorporated with stimulated Raman techniques such as femtosecond stimulated Raman spectroscopy (FSRS) and coherent anti-Stokes Raman spectroscopy (CARS). These techniques are capable of time-resolved measurement on the femtosecond and picosecond time scale and can be used to follow the dynamics of molecules reacting near plasmonic surfaces. We discuss the potential application of ultrafast SERS techniques to probe plasmon-mediated processes, such as H2 dissociation and solar steam production. Additionally, we discuss the possibilities for high sensitivity SERS sensing using these stimulated Raman spectroscopies.

Locking Lasers to RF in an Ultrafast FEL

International Nuclear Information System (INIS)

Wilcox, R.; Huang, G.; Doolittle, L.; White, W.; Frisch, J.; Coffee, R.

2010-01-01

Using a novel, phase-stabilized RF-over-fiber scheme, they transmit 3GHz over 300m with 27fs RMS error in 250kHz bandwidth over 12 hours, and phase lock a laser to enable ultrafast pump-probe experiments. Free-electron lasers (FELs) are capable of producing short-duration (< 10fs), high-energy X-ray pulses for a range of scientific applications. The recently activated Linac Coherent Light Source (LCLS) FEL facility at SLAC will support experiments which require synchronized light pulses for pump-probe schemes. They developed and operated a fiber optic RF transmission system to synchronize lasers to the emitted X-ray pulses, which was used to enable the first pump-probe experiments at the LCLS.

Electromechanical capacitor for energy transfer

International Nuclear Information System (INIS)

Carroll, T.A.; Chowdhuri, P.; Marshall, J.

1983-01-01

Inductive energy transfer between two magnets can be achieved with almost 100% efficiency with a transfer capacitor. However, the bulk and cost will be high, and reliability low if conventional capacitors are used. A homopolar machine, used as a capacitor, will be compact and economical. A homopolar machine was designed with counter-rotating copper disks completely immersed in a liquid metal (NaK-78) to work as a pulse capacitor. Absence of solid-brush collectors minimized wear and frictional losses. Wetting of the copper disks throughout the periphery by the liquid metal minimized the resistive losses at the collector interface. A liquid-metal collector would, however, introduce hydrodynamic and magnetohydrodynamic losses. The selected liquid metal, e.g., NaK-78 will produce the lowest of such losses among the available liquid metals. An electromechanical capacitor of this design was tested at various dc magnetic fields. Its measured capacitance was about 100 farads at a dc magnetic field of 1.15 tesla

Ultrafast gas switching experiments

International Nuclear Information System (INIS)

Frost, C.A.; Martin, T.H.; Patterson, P.E.; Rinehart, L.F.; Rohwein, G.J.; Roose, L.D.; Aurand, J.F.; Buttram, M.T.

1993-01-01

We describe recent experiments which studied the physics of ultrafast gas breakdown under the extreme overvoltages which occur when a high pressure gas switch is pulse charged to hundreds of kV in 1 ns or less. The highly overvolted peaking gaps produce powerful electromagnetic pulses with risetimes Khz at > 100 kV/m E field

Bridging the Radiative Transfer Models for Meteorology and Solar Energy Applications

Science.gov (United States)

Xie, Y.; Sengupta, M.

2017-12-01

Radiative transfer models are used to compute solar radiation reaching the earth surface and play an important role in both meteorology and solar energy studies. Therefore, they are designed to meet the needs of specialized applications. For instance, radiative transfer models for meteorology seek to provide more accurate cloudy-sky radiation compared to models used in solar energy that are geared towards accuracy in clear-sky conditions associated with the maximum solar resource. However, models for solar energy applications are often computationally faster, as the complex solution of the radiative transfer equation is parameterized by atmospheric properties that can be acquired from surface- or satellite-based observations. This study introduces the National Renewable Energy Laboratory's (NREL's) recent efforts to combine the advantages of radiative transfer models designed for meteorology and solar energy applictions. A fast all-sky radiation model, FARMS-NIT, was developed to efficiently compute narrowband all-sky irradiances over inclined photovoltaic (PV) panels. This new model utilizes the optical preperties from a solar energy model, SMARTS, to computes surface radiation by considering all possible paths of photon transmission and the relevent scattering and absorption attenuation. For cloudy-sky conditions, cloud bidirectional transmittance functions (BTDFs) are provided by a precomputed lookup table (LUT) by LibRadtran. Our initial results indicate that FARMS-NIT has an accuracy that is similar to LibRadtran, a highly accurate multi-stream model, but is significantly more efficient. The development and validation of this model will be presented.

Ultrafast magnetization dynamics

OpenAIRE

Woodford, Simon

2008-01-01

This thesis addresses ultrafast magnetization dynamics from a theoretical perspective. The manipulation of magnetization using the inverse Faraday effect has been studied, as well as magnetic relaxation processes in quantum dots. The inverse Faraday effect – the generation of a magnetic field by nonresonant, circularly polarized light – offers the possibility to control and reverse magnetization on a timescale of a few hundred femtoseconds. This is important both for the technological advant...

Tissue strain rate estimator using ultrafast IQ complex data

OpenAIRE

TERNIFI , Redouane; Elkateb Hachemi , Melouka; Remenieras , Jean-Pierre

2012-01-01

International audience; Pulsatile motion of brain parenchyma results from cardiac and breathing cycles. In this study, transient motion of brain tissue was estimated using an Aixplorer® imaging system allowing an ultrafast 2D acquisition mode. The strain was computed directly from the ultrafast IQ complex data using the extended autocorrelation strain estimator (EASE), which provides great SNRs regardless of depth. The EASE first evaluates the autocorrelation function at each depth over a set...

An ultrafast line-by-line algorithm for calculating spectral transmittance and radiance

International Nuclear Information System (INIS)

Tan, X.

2013-01-01

An ultrafast line-by-line algorithm for calculating spectral transmittance and radiance of gases is presented. The algorithm is based on fast convolution of the Voigt line profile using Fourier transform and a binning technique. The algorithm breaks a radiative transfer calculation into two steps: a one-time pre-computation step in which a set of pressure independent coefficients are computed using the spectral line information; a normal calculation step in which the Fourier transform coefficients of the optical depth are calculated using the line of sight information and the coefficients pre-computed in the first step, the optical depth is then calculated using an inverse Fourier transform and the spectral transmittance and radiance are calculated. The algorithm is significantly faster than line-by-line algorithms that do not employ special speedup techniques by a factor of 10 3 –10 6 . A case study of the 2.7 μm band of H 2 O vapor is presented. -- Highlights: •An ultrafast line-by-line model based on FFT and a binning technique is presented. •Computationally expensive calculations are factored out into a pre-computation step. •It is 10 3 –10 8 times faster than LBL algorithms that do not employ speedup techniques. •Good agreement with experimental data for the 2.7 μm band of H 2 O

Patellofemoral joint motion: Evaluation by ultrafast computed tomography

International Nuclear Information System (INIS)

Stanford, W.; Phelan, J.; Kathol, M.H.; Rooholamini, S.A.; El-Khoury, G.Y.; Palutsis, G.R.; Albright, J.P.

1988-01-01

Patellofemoral maltracking is a recognized cause of peripatellar pain. Clinicians currently rely on observation, palpation, and static radiographic images to evaluate the symptomatic patient. Ultrafast computed tomography (ultrafast CT) offers objective observations of the dynamic influences of muscle contraction on the patellofemoral joint as the knee is actively moved through a range of motion from 90 0 C flexion of full extension. This study reports our initial observations and establishes a range of normal values so that patients with a clinical suspicion of patellar maltracking may be evaluated. (orig./GDG)

Patellofemoral joint motion: Evaluation by ultrafast computed tomography

Energy Technology Data Exchange (ETDEWEB)

Stanford, W.; Phelan, J.; Kathol, M.H.; Rooholamini, S.A.; El-Khoury, G.Y.; Palutsis, G.R.; Albright, J.P.

1988-10-01

Patellofemoral maltracking is a recognized cause of peripatellar pain. Clinicians currently rely on observation, palpation, and static radiographic images to evaluate the symptomatic patient. Ultrafast computed tomography (ultrafast CT) offers objective observations of the dynamic influences of muscle contraction on the patellofemoral joint as the knee is actively moved through a range of motion from 90/sup 0/C flexion of full extension. This study reports our initial observations and establishes a range of normal values so that patients with a clinical suspicion of patellar maltracking may be evaluated. (orig./GDG).

Geometry effect on energy transfer rate in a coupled-quantum-well structure: nonlinear regime

International Nuclear Information System (INIS)

Salavati-fard, T; Vazifehshenas, T

2014-01-01

We study theoretically the effect of geometry on the energy transfer rate at nonlinear regime in a coupled-quantum-well system using the balance equation approach. To investigate comparatively the effect of both symmetric and asymmetric geometry, different structures are considered. The random phase approximation dynamic dielectric function is employed to include the contributions from both quasiparticle and plasmon excitations. Also, the short-range exchange interaction is taken into account through the Hubbard approximation. Our numerical results show that the energy transfer rate increases by increasing the well thicknesses in symmetric structures. Furthermore, by increasing spatial asymmetry, the energy transfer rate decreases for the electron temperature range of interest. From numerical calculations, it is obtained that the nonlinear energy transfer rate is proportional to the square of electron drift velocity in all structures and also, found that the influence of Hubbard local field correction on the energy transfer rate gets weaker by increasing the strength of applied electric field. (paper)