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Sample records for include exciton optics

  1. Nonboson treatment of excitonic nonlinearity in optically excited media

    International Nuclear Information System (INIS)

    Nguyen Ba An.

    1990-11-01

    The present article shortly reviews some recent results in the study of excitonic nonlinearity in optically excited media using a nonboson treatment for many-exciton systems. After a brief discussion of the exciton nonbosonity the closed commutation relations are given for exciton operators which hold for any exciton density and type. The nonboson treatment is then applied to the problems of intrinsic optical bistability and nonlinear polariton yielding quite interesting and new effects, e.g. new shapes of hysteresis loops of intrinsic optical bistability or anomalies of polariton dispersion. (author). 71 refs, 4 figs

  2. Excitonic optical bistability in n-type doped semiconductors

    International Nuclear Information System (INIS)

    Nguyen Ba An; Le Thi Cat Tuong

    1991-07-01

    A resonant monochromatic pump laser generates coherent excitons in an n-type doped semiconductor. Both exciton-exciton and exciton-donor interactions come into play. The former interaction can give rise to the appearance of optical bistability which is heavily influenced by the latter one. When optical bistability occurs at a fixed laser frequency both its holding intensity and hysteresis loop size are shown to decrease with increasing donor concentration. Two possibilities are suggested for experimentally determining one of the two parameters of the system - the exciton-donor coupling constant and the donor concentration, if the other parameter is known beforehand. (author). 36 refs, 2 figs

  3. Optical nutation in the exciton range of spectrum

    International Nuclear Information System (INIS)

    Khadzhi, P. I.; Vasiliev, V. V.

    2013-01-01

    Optical nutation in the exciton range of spectrum is studied in the mean field approximation taking into account exciton-photon and elastic exciton-exciton interactions. It is shown that the features of nutation development are determined by the initial exciton and photon densities, the resonance detuning, the nonlinearity parameter, and the initial phase difference. For nonzero initial exciton and photon concentrations, three regimes of temporal evolution of excitons and photons exist: periodic conversion of excitons to photons and vice versa, aperiodic conversion of photons to excitons, and the rest regime. In the rest regime, the initial exciton and photon densities are nonzero and do not change with time. The oscillation amplitudes and periods of particle densities determined by the system parameters are found. The exciton self-trapping and photon trapping appearing in the system at threshold values of the nonlinearity parameter were predicted. As this parameter increases, the oscillation amplitudes of the exciton and photon densities sharply change at the critical value of the nonlinearity parameter. These two phenomena are shown to be caused by the elastic exciton-exciton interaction, resulting in the dynamic concentration shift of the exciton level

  4. Magneto-optical quantum interferences in a system of spinor excitons

    Science.gov (United States)

    Kuan, Wen-Hsuan; Gudmundsson, Vidar

    2018-04-01

    In this work we investigate magneto-optical properties of two-dimensional semiconductor quantum-ring excitons with Rashba and Dresselhaus spin-orbit interactions threaded by a magnetic flux perpendicular to the plane of the ring. By calculating the excitonic Aharonov-Bohm spectrum, we study the Coulomb and spin-orbit effects on the Aharonov-Bohm features. From the light-matter interactions of the excitons, we find that for scalar excitons, there are open channels for spontaneous recombination resulting in a bright photoluminescence spectrum, whereas the forbidden recombination of dipolar excitons results in a dark photoluminescence spectrum. We investigate the generation of persistent charge and spin currents. The exploration of spin orientations manifests that by adjusting the strength of the spin-orbit interactions, the exciton can be constructed as a squeezed complex with specific spin polarization. Moreover, a coherently moving dipolar exciton acquires a nontrivial dual Aharonov-Casher phase, creating the possibility to generate persistent dipole currents and spin dipole currents. Our study reveals that in the presence of certain spin-orbit generated fields, the manipulation of the magnetic field provides a potential application for quantum-ring spinor excitons to be utilized in nano-scaled magneto-optical switches.

  5. Quasiparticle energies, excitons, and optical spectra of few-layer black phosphorus

    International Nuclear Information System (INIS)

    Tran, Vy; Fei, Ruixiang; Yang, Li

    2015-01-01

    We report first-principles GW–Bethe–Salpeter-equation (BSE) studies of excited-state properties of few-layer black phosphorus (BP) (phosphorene). With improved GW computational methods, we obtained converged quasiparticle band gaps and optical absorption spectra by the single-shot (G 0 W 0 ) procedure. Moreover, we reveal fine structures of anisotropic excitons, including the series of one-dimensional like wave functions, spin singlet–triplet splitting, and electron–hole binding energy spectra by solving BSE. An effective-mass model is employed to describe these electron–hole pairs, shedding light on estimating the exciton binding energy of anisotropic two-dimensional semiconductors without expensive ab initio simulations. Finally, the anisotropic optical response of BP is explained by using optical selection rules based on the projected single-particle density of states at band edges. (paper)

  6. Polarized excitons and optical activity in single-wall carbon nanotubes

    Science.gov (United States)

    Chang, Yao-Wen; Jin, Bih-Yaw

    2018-05-01

    The polarized excitons and optical activity of single-wall carbon nanotubes (SWNTs) are studied theoretically by π -electron Hamiltonian and helical-rotational symmetry. By taking advantage of the symmetrization, the single-particle energy and properties of a SWNT are characterized with the corresponding helical band structure. The dipole-moment matrix elements, magnetic-moment matrix elements, and the selection rules can also be derived. Based on different selection rules, the optical transitions can be assigned as the parallel-polarized, left-handed circularly-polarized, and right-handed circularly-polarized transitions, where the combination of the last two gives the cross-polarized transition. The absorption and circular dichroism (CD) spectra are simulated by exciton calculation. The calculated results are well comparable with the reported measurements. Built on the foundation, magnetic-field effects on the polarized excitons and optical activity of SWNTs are studied. Dark-bright exciton splitting and interband Faraday effect in the CD spectrum of SWNTs under an axial magnetic field are predicted. The Faraday rotation dispersion can be analyzed according to the selection rules of circular polarizations and the helical band structure.

  7. Optical Selection Rule of Excitons in Gapped Chiral Fermion Systems

    Science.gov (United States)

    Zhang, Xiaoou; Shan, Wen-Yu; Xiao, Di

    2018-02-01

    We show that the exciton optical selection rule in gapped chiral fermion systems is governed by their winding number w , a topological quantity of the Bloch bands. Specifically, in a CN-invariant chiral fermion system, the angular momentum of bright exciton states is given by w ±1 +n N with n being an integer. We demonstrate our theory by proposing two chiral fermion systems capable of hosting dark s -like excitons: gapped surface states of a topological crystalline insulator with C4 rotational symmetry and biased 3 R -stacked MoS2 bilayers. In the latter case, we show that gating can be used to tune the s -like excitons from bright to dark by changing the winding number. Our theory thus provides a pathway to electrical control of optical transitions in two-dimensional material.

  8. Exploring excitonic signal in optical conductivity of ZnO through first-order electron-hole vertex correction

    Science.gov (United States)

    Khoirunnisa, Humaira; Aziz Majidi, Muhammad

    2018-04-01

    The emergence of exitonic signal in the optical response of a wide band-gap semiconductor has been a common knowledge in physics. There have been numerous experimental studies exploring the important role of excitons on influencing both the transport and optical properties of the materials. Despite the existence of much information on excitonic effects, there has not been much literature that explores detailed theoretical explanation on how the exitonic signal appears and how it evolves with temperature. Here, we propose a theoretical study on the optical conductivity of ZnO, a well-known wide band-gap semiconductor that we choose as a case study. ZnO has been known to exhibit excitonic states in its optical spectra in the energy range of ∼3.13-3.41 eV, with a high exciton binding energy of ∼60 meV. An experimental study on ZnO in 2014 revealed such a signal in its optical conductivity spectrum. We present a theoretical investigation on the appearance of excitonic signal in optical conductivity of ZnO. We model the wurtzite ZnO within an 8-band k.p approximation. We calculate the optical conductivity by incorporating the first-order vertex correction derived from the Feynman diagrams. Our calculation up to the first-order correction spectrum qualitatively confirms the existence of excitons in wurtzite ZnO.

  9. Radiative control of dark excitons at room temperature by nano-optical antenna-tip Purcell effect

    Science.gov (United States)

    Park, Kyoung-Duck; Jiang, Tao; Clark, Genevieve; Xu, Xiaodong; Raschke, Markus B.

    2018-01-01

    Excitons, Coulomb-bound electron-hole pairs, are elementary photo-excitations in semiconductors that can couple to light through radiative relaxation. In contrast, dark excitons (XD) show anti-parallel spin configuration with generally forbidden radiative emission. Because of their long lifetimes, these dark excitons are appealing candidates for quantum computing and optoelectronics. However, optical read-out and control of XD states has remained challenging due to their decoupling from light. Here, we present a tip-enhanced nano-optical approach to induce, switch and programmably modulate the XD emission at room temperature. Using a monolayer transition metal dichalcogenide (TMD) WSe2 on a gold substrate, we demonstrate 6 × 105-fold enhancement in dark exciton photoluminescence quantum yield achieved through coupling of the antenna-tip to the dark exciton out-of-plane optical dipole moment, with a large Purcell factor of ≥2 × 103 of the tip-sample nano-cavity. Our approach provides a facile way to harness excitonic properties in low-dimensional semiconductors offering new strategies for quantum optoelectronics.

  10. Optical spectroscopy and imaging of the higher energy excitons and bandgap of monolayer MoS2

    Science.gov (United States)

    Borys, Nicholas; Bao, Wei; Barnard, Edward; Ko, Changhyun; Tongay, Sefaatin; Wu, Junqiao; Yang, Li; Schuck, P. James

    Monolayer MoS2 (ML-MoS2) exhibits a rich manifold of excitons that dictate optoelectronic performance and functionality. Disentangling these states, which include the quasi-particle bandgap, is critical for developing 2D optoelectronic devices that operate beyond the optical bandgap. Whereas photoluminescence (PL) spectroscopy only probes the lowest-energy radiative state and absorption spectroscopy fails to discriminate energetically degenerate states, photoluminescence excitation (PLE) spectroscopy selectively probes only the excited states that thermalize to the emissive ground state exciton. Using PLE spectroscopy of ML-MoS2, we identify the Rydberg series of the exciton A and exciton B states as well as signatures of the quasi-particle bandgap and coupling between the indirect C exciton and the lowest-energy A exciton, which have eluded previous PLE studies. The assignment of these states is confirmed with density functional theory. Mapping the PLE spectrum reveals spatial variations of the higher-energy exciton manifold and quasi-particle bandgap which mirror the heterogeneity in the PL but also indicate variations in local exciton thermalization processes and chemical potentials.

  11. The excitonic insulator route through a dynamical phase transition induced by an optical pulse

    Energy Technology Data Exchange (ETDEWEB)

    Brazovskii, S., E-mail: brazov@lptms.u-psud.fr [Université Paris-Saclay, LPTMS, CNRS, Univ. Paris-sud (France); Kirova, N. [Université Paris-Saclay, LPS, CNRS, Univ. Paris-sud (France)

    2016-03-15

    We consider a dynamical phase transition induced by a short optical pulse in a system prone to thermodynamical instability. We address the case of pumping to excitons whose density contributes directly to the order parameter. To describe both thermodynamic and dynamic effects on equal footing, we adopt a view of the excitonic insulator for the phase transition and suggest a formation of the Bose condensate for the pumped excitons. The work is motivated by experiments in donor–acceptor organic compounds with a neutral- ionic phase transition coupled to the spontaneous lattice dimerization and to charge transfer excitons. The double nature of the ensemble of excitons leads to an intricate time evolution, in particular, to macroscopic quantum oscillations from the interference between the Bose condensate of excitons and the ground state of the excitonic insulator. The coupling of excitons and the order parameter also leads to self-trapping of their wave function, akin to self-focusing in optics. The locally enhanced density of excitons can surpass a critical value to trigger the phase transformation, even if the mean density is below the required threshold. The system is stratified in domains that evolve through dynamical phase transitions and sequences of merging. The new circumstances in experiments and theory bring to life, once again, some remarkable inventions made by L.V. Keldysh.

  12. Exciton scattering approach for optical spectra calculations in branched conjugated macromolecules

    International Nuclear Information System (INIS)

    Li, Hao; Wu, Chao; Malinin, Sergey V.; Tretiak, Sergei; Chernyak, Vladimir Y.

    2016-01-01

    The exciton scattering (ES) technique is a multiscale approach based on the concept of a particle in a box and developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, electronic excitations in molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph whose edges and nodes stand for the molecular linear segments and vertices, respectively. Exciton propagation on the linear segments is characterized by the exciton dispersion, whereas exciton scattering at the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized “particle in a box” problems on the graph that represents the molecule. Similarly, unique energy-dependent ES dipolar parameters permit calculations of the corresponding oscillator strengths, thus, completing optical spectra modeling. Both the energetic and dipolar parameters can be extracted from quantum-chemical computations in small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within a considered molecular family could be performed with negligible numerical effort. We demonstrate the ES method application to molecular families of branched conjugated phenylacetylenes and ladder poly-para-phenylenes, as well as structures with electron donor and acceptor chemical substituents. Time-dependent density functional theory (TD-DFT) is used as a reference model for electronic structure. The ES calculations accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

  13. Exciton scattering approach for optical spectra calculations in branched conjugated macromolecules

    Science.gov (United States)

    Li, Hao; Wu, Chao; Malinin, Sergey V.; Tretiak, Sergei; Chernyak, Vladimir Y.

    2016-12-01

    The exciton scattering (ES) technique is a multiscale approach based on the concept of a particle in a box and developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, electronic excitations in molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph whose edges and nodes stand for the molecular linear segments and vertices, respectively. Exciton propagation on the linear segments is characterized by the exciton dispersion, whereas exciton scattering at the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized "particle in a box" problems on the graph that represents the molecule. Similarly, unique energy-dependent ES dipolar parameters permit calculations of the corresponding oscillator strengths, thus, completing optical spectra modeling. Both the energetic and dipolar parameters can be extracted from quantum-chemical computations in small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within a considered molecular family could be performed with negligible numerical effort. We demonstrate the ES method application to molecular families of branched conjugated phenylacetylenes and ladder poly-para-phenylenes, as well as structures with electron donor and acceptor chemical substituents. Time-dependent density functional theory (TD-DFT) is used as a reference model for electronic structure. The ES calculations accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

  14. Exciton scattering approach for optical spectra calculations in branched conjugated macromolecules

    Energy Technology Data Exchange (ETDEWEB)

    Li, Hao [Department of Chemistry, University of Houston, Houston, TX 77204 (United States); Wu, Chao [Electronic Structure Lab, Center of Microscopic Theory and Simulation, Frontier Institute of Science and Technology, Xian Jiaotong University, Xian 710054 (China); Malinin, Sergey V. [Department of Chemistry, Wayne State University, 5101 Cass Avenue, Detroit, MI 48202 (United States); Tretiak, Sergei, E-mail: serg@lanl.gov [Theoretical Division and Center for Nonlinear Studies, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Center for Integrated Nanotechnologies, Los Alamos National Laboratory, Los Alamos, NM 87545 (United States); Chernyak, Vladimir Y., E-mail: chernyak@chem.wayne.edu [Department of Chemistry, Wayne State University, 5101 Cass Avenue, Detroit, MI 48202 (United States)

    2016-12-20

    The exciton scattering (ES) technique is a multiscale approach based on the concept of a particle in a box and developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, electronic excitations in molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph whose edges and nodes stand for the molecular linear segments and vertices, respectively. Exciton propagation on the linear segments is characterized by the exciton dispersion, whereas exciton scattering at the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized “particle in a box” problems on the graph that represents the molecule. Similarly, unique energy-dependent ES dipolar parameters permit calculations of the corresponding oscillator strengths, thus, completing optical spectra modeling. Both the energetic and dipolar parameters can be extracted from quantum-chemical computations in small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within a considered molecular family could be performed with negligible numerical effort. We demonstrate the ES method application to molecular families of branched conjugated phenylacetylenes and ladder poly-para-phenylenes, as well as structures with electron donor and acceptor chemical substituents. Time-dependent density functional theory (TD-DFT) is used as a reference model for electronic structure. The ES calculations accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

  15. Optical orientation and alignment of excitons in ensembles of inorganic perovskite nanocrystals

    OpenAIRE

    Nestoklon, M. O.; Goupalov, S. V.; Dzhioev, R. I.; Ken, O. S.; Korenev, V. L.; Kusrayev, Yu. G.; Sapega, V. F.; de Weerd, C.; Gomez, L.; Gregorkiewicz, T.; Lin, Junhao; Suenaga, Kazutomo; Fujiwara, Yasufumi; Matyushkin, L. B.; Yassievich, I. N.

    2018-01-01

    We demonstrate the optical orientation and alignment of excitons in a two-dimensional layer of CsPbI$_3$ perovskite nanocrystals prepared by colloidal synthesis and measure the anisotropic exchange splitting of exciton levels in the nanocrystals. From the experimental data at low temperature (2K), we obtain the average value of anisotropic splitting of bright exciton states of the order of 120{\\mu}eV. Our calculations demonstrate that there is a significant contribution to the splitting due t...

  16. New nonlinear optical effect: self-reflection phenomenon due to exciton-biexciton-light interaction in semiconductors

    Science.gov (United States)

    Khadzhi, P. I.; Lyakhomskaya, K. D.; Nadkin, L. Y.; Markov, D. A.

    2002-05-01

    The characteristic peculiarities of the self-reflection of a strong electromagnetic wave in a system of coherent excitons and biexcitons due to the exciton-photon interaction and optical exciton-biexciton conversion in semiconductors were investigated as one of the manifestations of nonlinear optical Stark-effect. It was found that a monotonously decreasing standing wave with an exponential decreasing spatial tail is formed in the semiconductor. Under the action of the field of a strong pulse, an optically homogeneous medium is converted, into the medium with distributed feedback. The appearance of the spatially separated narrow pears of the reflective index, extinction and reflection coefficients is predicted.

  17. Polarised two-photon excitation of quantum well excitons for manipulation of optically pumped terahertz lasers

    Energy Technology Data Exchange (ETDEWEB)

    Slavcheva, G., E-mail: gsk23@bath.ac.uk [Blackett Laboratory, Imperial College London, Prince Consort Road, London SW7 2AZ (United Kingdom); Kavokin, A.V., E-mail: A.Kavokin@soton.ac.uk [School of Physics and Astronomy, University of Southampton, Highfield, Southampton SO17 1BJ (United Kingdom); Spin Optics Laboratory, St. Petersburg State University, 1, Ulyanovskaya 198504 (Russian Federation)

    2014-11-15

    Optical pumping of excited exciton states in a semiconductor quantum well embedded in a microcavity is a tool for realisation of ultra-compact terahertz (THz) lasers based on stimulated optical transition between excited (2p) and ground (1s) exciton state. We show that the probability of two-photon absorption by a 2p-exciton is strongly dependent on the polarisation of both pumping photons. Five-fold variation of the threshold power for terahertz lasing by switching from circular to co-linear pumping is predicted. We identify photon polarisation configurations for achieving maximum THz photon generation quantum efficiency.

  18. Enhancement of nonlinear optical response of weakly confined excitons in GaAs thin films by spectrally rectangle-shape-pulse-excitation

    International Nuclear Information System (INIS)

    Kojima, O; Isu, T; Ishi-Hayase, J; Sasaki, M; Tsuchiya, M

    2007-01-01

    We report the enhancement of the nonlinear optical response of the weakly confined excitons with use of spectrally rectangular pulse. The nonlinear optical response was investigated as a function of excitation energy by a degenerate four-wave-mixing (DFWM) technique. In the case that the laser pulse with the controlled spectral shape excites the plural exciton states simultaneously, the DFWM signal intensity is enhanced by a factor of two in comparison with the intensity under the excitation of a single exciton state. This enhancement is caused by the superposition of the nonlinear optical responses from the plural exciton states

  19. Stark effect of optical properties of excitons in a quantum nanorod with parabolic confinement

    Energy Technology Data Exchange (ETDEWEB)

    Lyo, S.K., E-mail: sklyo@uci.edu

    2014-01-15

    We study the quantum Stark effect of optical properties of a quasi-one-dimensional quantum rod with parabolic confinement. Interplays between the competing/cooperative forces from confinement, electron–hole (e–h) attraction, and an external field are examined by studying the binding energy, the oscillator strength, and the root-mean-square (RMS) average of the e–h separation in a nonlinear electric field. In a long rod with weak confinement, the e–h interaction dominates over the confinement effect, yielding an abrupt drop of the exciton binding energy, oscillator strength, and a sudden increase of the RMS average e–h separation as the excitons are dissociated at the threshold field as the field increases. The exciton-dissociation transition is gradual in a short rod, where the confinement force dominates over the e–h attraction. We show that a DC field can induce an optically active excited exciton state in a narrow field range, causing a sharp peak in the oscillator strength and a dip in the RMS average of the e–h separation as the field increases. The Stark effects are also investigated as a function of the linear confinement length (i.e., rod length) at fixed fields. -- Highlights: • Study the dependence of optical properties of nanorods on the rod size and field. • Study the interplay between forces of confinement, Coulomb attraction, and field. • A strong field induces an optically active excited state observed in quantum dots.

  20. Optical nonlinearity and bistability in the bound exciton energy range of CdS

    International Nuclear Information System (INIS)

    Hoenig, T.; Gutowski, J.

    1988-01-01

    Under high excitation conditions thick CdS samples show pronounced broad-band nonlinear transmission in the bound exciton region and up to a wavelength of about 515 nm at cryo-temperatures. This behavior is only explainable in a model based on impurity neutralization and bound exciton creation. The suitability of these nonlinearities to yield optical bistability will be shown. Bistable operation is investigated in dependence of crystal thickness, impurity concentration, excitation density, wavelength, and temperature. A strong correlation to acceptor-bound exciton generation is obtained, and the explanation of this bistable operation fits well with that of the above mentioned transmission behavior. (author)

  1. Intense coherent longitudinal optical phonons in CuI thin films under exciton-excitation conditions

    International Nuclear Information System (INIS)

    Kojima, O.; Mizoguchi, K.; Nakayama, M..

    2005-01-01

    We have investigated the dynamical properties of the coherent longitudinal optical (LO) phonon in CuI thin films grown on a NaCl substrate by vacuum deposition. The intense coherent LO phonon in the CuI thin film is observed under the exciton-excitation conditions. Moreover, the pump-energy dependence of the amplitude of the coherent LO phonon shows peaks at the heavy-hole and light-hole exciton energies. The enhancement of the coherent LO phonon under the exciton-resonance condition is much larger than that in an ordinary semiconductor quantum well system such as a GaAs/AlAs one. These facts demonstrate that the intense coherent LO phonon is generated under the exciton-excitation condition in a material with a strong exciton-phonon interaction such as CuI

  2. Excitons in insulators

    International Nuclear Information System (INIS)

    Grasser, R.; Scharmann, A.

    1983-01-01

    This chapter investigates absorption, reflectivity, and intrinsic luminescence spectra of free and/or self-trapped (localized) excitons in alkali halides and rare gas solids. Introduces the concepts underlying the Wannier-Mott and Frenkel exciton models, two extreme pictures of an exciton in crystalline materials. Discusses the theoretical and experimental background; excitons in alkali halides; and excitons in rare gas solids. Shows that the intrinsic optical behavior of wide gap insulators in the range of the fundamental absorption edge is controlled by modified Wannier-Mott excitons. Finds that while that alkali halides only show free and relaxed molecular-like exciton emission, in rare gas crystals luminescence due to free, single and double centered localized excitons is observed. Indicates that the simultaneous existence of free and self-trapped excitons in these solid requires an energy barrier for self-trapping

  3. Optical and Excitonic Properties of Atomically Thin Transition-Metal Dichalcogenides

    Science.gov (United States)

    Berkelbach, Timothy C.; Reichman, David R.

    2018-03-01

    Starting with the isolation of a single sheet of graphene, the study of layered materials has been one of the most active areas of condensed matter physics, chemistry, and materials science. Single-layer transition-metal dichalcogenides are direct-gap semiconducting analogs of graphene that exhibit novel electronic and optical properties. These features provide exciting opportunities for the discovery of both new fundamental physical phenomena as well as innovative device platforms. Here, we review the progress associated with the creation and use of a simple microscopic framework for describing the optical and excitonic behavior of few-layer transition-metal dichalcogenides, which is based on symmetry, band structure, and the effective interactions between charge carriers in these materials. This approach provides an often quantitative account of experiments that probe the physics associated with strong electron–hole interactions in these quasi two-dimensional systems and has been successfully employed by many groups to both describe and predict emergent excitonic behavior in these layered semiconducting systems.

  4. Nonlinear optical spectra having characteristics of Fano interferences in coherently coupled lowest exciton biexciton states in semiconductor quantum dots

    Directory of Open Access Journals (Sweden)

    Hideki Gotoh

    2014-10-01

    Full Text Available Optical nonlinear effects are examined using a two-color micro-photoluminescence (micro-PL method in a coherently coupled exciton-biexciton system in a single quantum dot (QD. PL and photoluminescence excitation spectroscopy (PLE are employed to measure the absorption spectra of the exciton and biexciton states. PLE for Stokes and anti-Stokes PL enables us to clarify the nonlinear optical absorption properties in the lowest exciton and biexciton states. The nonlinear absorption spectra for excitons exhibit asymmetric shapes with peak and dip structures, and provide a distinct contrast to the symmetric dip structures of conventional nonlinear spectra. Theoretical analyses with a density matrix method indicate that the nonlinear spectra are caused not by a simple coherent interaction between the exciton and biexciton states but by coupling effects among exciton, biexciton and continuum states. These results indicate that Fano quantum interference effects appear in exciton-biexciton systems at QDs and offer important insights into their physics.

  5. Confined exciton spectroscopy

    International Nuclear Information System (INIS)

    Torres, Clivia M.S.

    1998-01-01

    Full text: In this work, the exciton is considered as a sensor of the electronic and optical properties of materials such as semiconductors, which have size compared to the exciton De Broglie wavelength, approximately 20 nm, depending on the semiconductor. Examples of electron-phonon, electron-electron, photon-electron, exciton-polariton, phonon-plasmon, are presented, under different confinement conditions such as quantum wells, superlattices

  6. Plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites

    Science.gov (United States)

    Bityurin, N.; Ermolaev, N.; Smirnov, A. A.; Afanasiev, A.; Agareva, N.; Koryukina, T.; Bredikhin, V.; Kamensky, V.; Pikulin, A.; Sapogova, N.

    2016-03-01

    UV irradiation of materials consisting of a polymer matrix that possesses precursors of different kinds can result in creation of nanoparticles within the irradiated domains. Such photoinduced nanocomposites are promising for photonic applications due to the strong alteration of their optical properties compared to initial non-irradiated materials. We report our results on the synthesis and investigation of plasmonic, excitonic and exciton-plasmonic photoinduced nanocomposites. Plasmonic nanocomposites contain metal nanoparticles of noble metals with a pronounced plasmon resonance. Excitonic nanocomposites possess semiconductor nanoclusters (quantum dots). We consider the CdS-Au pair because the luminescent band of CdS nanoparticles enters the plasmon resonance band of gold nanoparticles. The obtaining of such particles within the same composite materials is promising for the creation of media with exciton-plasmon resonance. We demonstrate that it is possible to choose appropriate precursor species to obtain the initially transparent poly(methyl methacrylate) (PMMA) films containing both types of these molecules either separately or together. Proper irradiation of these materials by a light-emitting diode operating at the wavelength of 365 nm provides material alteration demonstrating light-induced optical absorption and photoluminescent properties typical for the corresponding nanoparticles. Thus, an exciton-plasmonic photoinduced nanocomposite is obtained. It is important that here we use the precursors that are different from those usually employed.

  7. Exciton diamagnetic shift and optical properties in CdSe nanocrystal quantum dots in magnetic fields

    Science.gov (United States)

    Wu, Shudong; Cheng, Liwen

    2018-04-01

    The magnetic field dependence of the optical properties of CdSe nanocrystal quantum dots (NQDs) is investigated theoretically using a perturbation method within the effective-mass approximation. The results show that the magnetic field lifts the degeneracy of the electron (hole) states. A blue-shift in the absorption spectra of m ≥ 0 exciton states is observed while the absorption peak of m attributed to the interplay of the orbital Zeeman effect and the additive confinement induced by the magnetic field. The excitonic absorption coefficient is almost independent of B in the strong confinement regime. The applied magnetic field causes the splitting of degenerated exciton states, resulting in the new absorption peaks. Based on the first-order perturbation theory, we propose the analytical expressions for the exciton binding energy, exciton transition energy and exciton diamagnetic shift of 1s, 1p-1, 1p0, 1p1, 1d-2, 1d-1, 1d0, 1d1, 1d2 and 2s exciton states on the applied magnetic field in the strong confinement regime.

  8. Atomic lattice excitons: from condensates to crystals

    International Nuclear Information System (INIS)

    Kantian, A; Daley, A J; Toermae, P; Zoller, P

    2007-01-01

    We discuss atomic lattice excitons (ALEs), bound particle-hole pairs formed by fermionic atoms in two bands of an optical lattice. Such a system provides a clean set-up, with tunable masses and interactions, to study fundamental properties of excitons including exciton condensation. We also find that for a large effective mass ratio between particles and holes, effective long-range interactions can mediate the formation of an exciton crystal, for which superfluidity is suppressed. Using a combination of mean-field treatments, bosonized theory based on a Born-Oppenheimer approximation, and one-dimensional (1D) numerical computation, we discuss the properties of ALEs under varying conditions, and discuss in particular their preparation and measurement

  9. Atomic lattice excitons: from condensates to crystals

    Energy Technology Data Exchange (ETDEWEB)

    Kantian, A [Institute for Quantum Optics and Quantum Information of the Austrian Academy of Sciences, A-6020 Innsbruck (Austria); Daley, A J [Institute for Quantum Optics and Quantum Information of the Austrian Academy of Sciences, A-6020 Innsbruck (Austria); Toermae, P [Nanoscience Center, Department of Physics, University of Jyvaeskylae, PO Box 35, FIN-40014 (Finland); Zoller, P [Institute for Quantum Optics and Quantum Information of the Austrian Academy of Sciences, A-6020 Innsbruck (Austria)

    2007-11-15

    We discuss atomic lattice excitons (ALEs), bound particle-hole pairs formed by fermionic atoms in two bands of an optical lattice. Such a system provides a clean set-up, with tunable masses and interactions, to study fundamental properties of excitons including exciton condensation. We also find that for a large effective mass ratio between particles and holes, effective long-range interactions can mediate the formation of an exciton crystal, for which superfluidity is suppressed. Using a combination of mean-field treatments, bosonized theory based on a Born-Oppenheimer approximation, and one-dimensional (1D) numerical computation, we discuss the properties of ALEs under varying conditions, and discuss in particular their preparation and measurement.

  10. Excitons in atomically thin 2D semiconductors and their applications

    Science.gov (United States)

    Xiao, Jun; Zhao, Mervin; Wang, Yuan; Zhang, Xiang

    2017-06-01

    The research on emerging layered two-dimensional (2D) semiconductors, such as molybdenum disulfide (MoS2), reveals unique optical properties generating significant interest. Experimentally, these materials were observed to host extremely strong light-matter interactions as a result of the enhanced excitonic effect in two dimensions. Thus, understanding and manipulating the excitons are crucial to unlocking the potential of 2D materials for future photonic and optoelectronic devices. In this review, we unravel the physical origin of the strong excitonic effect and unique optical selection rules in 2D semiconductors. In addition, control of these excitons by optical, electrical, as well as mechanical means is examined. Finally, the resultant devices such as excitonic light emitting diodes, lasers, optical modulators, and coupling in an optical cavity are overviewed, demonstrating how excitons can shape future 2D optoelectronics.

  11. Dark excitons in transition metal dichalcogenides

    Science.gov (United States)

    Malic, Ermin; Selig, Malte; Feierabend, Maja; Brem, Samuel; Christiansen, Dominik; Wendler, Florian; Knorr, Andreas; Berghäuser, Gunnar

    2018-01-01

    Monolayer transition metal dichalcogenides (TMDs) exhibit a remarkably strong Coulomb interaction that manifests in tightly bound excitons. Due to the complex electronic band structure exhibiting several spin-split valleys in the conduction and valence band, dark excitonic states can be formed. They are inaccessibly by light due to the required spin-flip and/or momentum transfer. The relative position of these dark states with respect to the optically accessible bright excitons has a crucial impact on the emission efficiency of these materials and thus on their technological potential. Based on the solution of the Wannier equation, we present the excitonic landscape of the most studied TMD materials including the spectral position of momentum- and spin-forbidden excitonic states. We show that the knowledge of the electronic dispersion does not allow to conclude about the nature of the material's band gap since excitonic effects can give rise to significant changes. Furthermore, we reveal that an exponentially reduced photoluminescence yield does not necessarily reflect a transition from a direct to a nondirect gap material, but can be ascribed in most cases to a change of the relative spectral distance between bright and dark excitonic states.

  12. Interplay of Cu and oxygen vacancy in optical transitions and screening of excitons in ZnO:Cu films

    International Nuclear Information System (INIS)

    Darma, Yudi; Rusydi, Andrivo; Seng Herng, Tun; Marlina, Resti; Fauziah, Resti; Ding, Jun

    2014-01-01

    We study room temperature optics and electronic structures of ZnO:Cu films as a function of Cu concentration using a combination of spectroscopic ellipsometry, photoluminescence, and ultraviolet-visible absorption spectroscopy. Mid-gap optical states, interband transitions, and excitons are observed and distinguishable. We argue that the mid-gap states are originated from interactions of Cu and oxygen vacancy (Vo). They are located below conduction band (Zn4s) and above valence band (O2p) promoting strong green emission and narrowing optical band gap. Excitonic states are screened and its intensities decrease upon Cu doping. Our results show the importance of Cu and Vo driving the electronic structures and optical transitions in ZnO:Cu films

  13. Interplay of Cu and oxygen vacancy in optical transitions and screening of excitons in ZnO:Cu films

    Science.gov (United States)

    Darma, Yudi; Seng Herng, Tun; Marlina, Resti; Fauziah, Resti; Ding, Jun; Rusydi, Andrivo

    2014-02-01

    We study room temperature optics and electronic structures of ZnO:Cu films as a function of Cu concentration using a combination of spectroscopic ellipsometry, photoluminescence, and ultraviolet-visible absorption spectroscopy. Mid-gap optical states, interband transitions, and excitons are observed and distinguishable. We argue that the mid-gap states are originated from interactions of Cu and oxygen vacancy (Vo). They are located below conduction band (Zn4s) and above valence band (O2p) promoting strong green emission and narrowing optical band gap. Excitonic states are screened and its intensities decrease upon Cu doping. Our results show the importance of Cu and Vo driving the electronic structures and optical transitions in ZnO:Cu films.

  14. Electronic structure and optical properties of triangular GaAs/AlGaAs quantum dots: Exciton and impurity states

    International Nuclear Information System (INIS)

    Tiutiunnyk, A.; Akimov, V.; Tulupenko, V.; Mora-Ramos, M.E.; Kasapoglu, E.; Ungan, F.; Sökmen, I.

    2016-01-01

    Electronic structure and optical properties in equilateral triangular GaAs/Al_0_._3Ga_0_._7As quantum dots are studied extensively. The effects of donor and acceptor impurity atoms positioned in the orthocenter of the triangle, as well as of the external DC electric field are taken into account. Binding energies of the impurity, exciton energies, interband photoluminescence peak positions as well as linear and non-linear optical properties in THz range caused by transitions between excitonic states are calculated and discussed.

  15. Optical nonlinearities of excitonic states in atomically thin 2D transition metal dichalcogenides

    Energy Technology Data Exchange (ETDEWEB)

    Soh, Daniel Beom Soo [Sandia National Lab. (SNL-CA), Livermore, CA (United States). Proliferation Signatures Discovery and Exploitation Department

    2017-08-01

    We calculated the optical nonlinearities of the atomically thin monolayer transition metal dichalcogenide material (particularly MoS2), particularly for those linear and nonlinear transition processes that utilize the bound exciton states. We adopted the bound and the unbound exciton states as the basis for the Hilbert space, and derived all the dynamical density matrices that provides the induced current density, from which the nonlinear susceptibilities can be drawn order-by-order via perturbative calculations. We provide the nonlinear susceptibilities for the linear, the second-harmonic, the third-harmonic, and the kerr-type two-photon processes.

  16. Excitonic Effects in Methylammonium Lead Halide Perovskites

    Energy Technology Data Exchange (ETDEWEB)

    Beard, Matthew C [National Renewable Energy Laboratory (NREL), Golden, CO (United States); Chen, Xihan [National Renewable Energy Laboratory (NREL), Golden, CO (United States); Lu, Haipeng [National Renewable Energy Laboratory (NREL), Golden, CO (United States); Yang, Ye [National Renewable Energy Laboratory (NREL), Golden, CO (United States)

    2018-05-01

    The exciton binding energy in methylammonium lead iodide (MAPbI3) is about 10 meV, around 1/3 of the available thermal energy (kBT ~ 26 meV) at room temperature. Thus, exciton populations are not stable at room temperature at moderate photoexcited carrier densities. However, excitonic resonances dominate the absorption onset. Furthermore, these resonances determine the transient absorbance and transient reflectance spectra. The exciton binding energy is a reflection of the Coulomb interaction energy between photoexcited electrons and holes. As such, it serves as a marker for the strength of electron/hole interactions and impacts a variety of phenomena, such as, absorption, radiative recombination, and Auger recombination. In this Perspective, we discuss the role of excitons and excitonic resonances in the optical properties of lead-halide perovskite semiconductors. Finally, we discuss how the strong light-matter interactions induce an optical stark effect splitting the doubly spin degenerate ground exciton states and are easily observed at room temperature.

  17. Electronic structure and optical properties of triangular GaAs/AlGaAs quantum dots: Exciton and impurity states

    Energy Technology Data Exchange (ETDEWEB)

    Tiutiunnyk, A. [Grupo de Materia Condensada-UdeA, Instituto de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín (Colombia); Department of Physics, Donbass State Engineering Academy, Shkadinova 72, 84313 Kramatorsk (Ukraine); Akimov, V. [Grupo de Materia Condensada-UdeA, Instituto de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín (Colombia); Department of Physics, Donbass State Engineering Academy, Shkadinova 72, 84313 Kramatorsk (Ukraine); Universidad de Medellín, Carrera 87 No 30-65 Medellín (Colombia); Tulupenko, V. [Grupo de Materia Condensada-UdeA, Instituto de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín (Colombia); Department of Physics, Donbass State Engineering Academy, Shkadinova 72, 84313 Kramatorsk (Ukraine); Mora-Ramos, M.E. [Centro de Investigación en Ciencias, Instituto de Investigación en Ciencias Básicas y Aplicadas, Universidad Autónoma del Estado de Morelos, Av. Universidad 1001, CP 62209 Cuernavaca, Morelos (Mexico); Kasapoglu, E. [Cumhuriyet University, Physics Department, 58140 Sivas (Turkey); Ungan, F. [Cumhuriyet University, Faculty of Technology, Deparment of Optical Engineering, 58140 Sivas (Turkey); Sökmen, I. [Department of Physics, Dokuz Eylül University, 35160 Buca, İzmir (Turkey); and others

    2016-03-01

    Electronic structure and optical properties in equilateral triangular GaAs/Al{sub 0.3}Ga{sub 0.7}As quantum dots are studied extensively. The effects of donor and acceptor impurity atoms positioned in the orthocenter of the triangle, as well as of the external DC electric field are taken into account. Binding energies of the impurity, exciton energies, interband photoluminescence peak positions as well as linear and non-linear optical properties in THz range caused by transitions between excitonic states are calculated and discussed.

  18. Optically Discriminating Carrier-Induced Quasiparticle Band Gap and Exciton Energy Renormalization in Monolayer MoS_{2}.

    Science.gov (United States)

    Yao, Kaiyuan; Yan, Aiming; Kahn, Salman; Suslu, Aslihan; Liang, Yufeng; Barnard, Edward S; Tongay, Sefaattin; Zettl, Alex; Borys, Nicholas J; Schuck, P James

    2017-08-25

    Optoelectronic excitations in monolayer MoS_{2} manifest from a hierarchy of electrically tunable, Coulombic free-carrier and excitonic many-body phenomena. Investigating the fundamental interactions underpinning these phenomena-critical to both many-body physics exploration and device applications-presents challenges, however, due to a complex balance of competing optoelectronic effects and interdependent properties. Here, optical detection of bound- and free-carrier photoexcitations is used to directly quantify carrier-induced changes of the quasiparticle band gap and exciton binding energies. The results explicitly disentangle the competing effects and highlight longstanding theoretical predictions of large carrier-induced band gap and exciton renormalization in two-dimensional semiconductors.

  19. Optically Discriminating Carrier-Induced Quasiparticle Band Gap and Exciton Energy Renormalization in Monolayer MoS2

    Science.gov (United States)

    Yao, Kaiyuan; Yan, Aiming; Kahn, Salman; Suslu, Aslihan; Liang, Yufeng; Barnard, Edward S.; Tongay, Sefaattin; Zettl, Alex; Borys, Nicholas J.; Schuck, P. James

    2017-08-01

    Optoelectronic excitations in monolayer MoS2 manifest from a hierarchy of electrically tunable, Coulombic free-carrier and excitonic many-body phenomena. Investigating the fundamental interactions underpinning these phenomena—critical to both many-body physics exploration and device applications—presents challenges, however, due to a complex balance of competing optoelectronic effects and interdependent properties. Here, optical detection of bound- and free-carrier photoexcitations is used to directly quantify carrier-induced changes of the quasiparticle band gap and exciton binding energies. The results explicitly disentangle the competing effects and highlight longstanding theoretical predictions of large carrier-induced band gap and exciton renormalization in two-dimensional semiconductors.

  20. Triplet exciton diffusion in organic semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Koehler, Anna [Department of Physics, University of Bayreuth (Germany)

    2010-07-01

    Efficient triplet exciton emission has allowed improved operation of organic light-emitting diodes (LEDs). To enhance the device performance, it is necessary to understand what governs the motion of triplet excitons through the organic semiconductor. We use a series of poly(p-phenylene)-type conjugated polymers and oligomers of variable degree of molecular distortion (i.e. polaron formation) and energetic disorder as model systems to study the Dexter-type triplet exciton diffusion in thin films. We show that triplet diffusion can be quantitatively described in the framework of a Holstein small polaron model (Marcus theory) that is extended to include contributions from energetic disorder. The model predicts a tunnelling process at low temperatures followed by a thermally activated hopping process above a transition temperature. In contrast to charge transfer, the activation energy required for triplet exciton transfer can be deduced from the optical spectra. We discuss the implications for device architecture.

  1. Correction of the exciton Bohr radius in monolayer transition metal dichalcogenides

    Science.gov (United States)

    Li, Run-Ze; Dong, Xi-Ying; Li, Zhi-Qing; Wang, Zi-Wu

    2018-07-01

    We theoretically investigate the correction of exciton Bohr radius in monolayer transition metal dichalcogenides (TMDCs) on different polar substrates arising from the exciton-optical phonon coupling, in which both the intrinsic longitudinal optical phonon and surface optical phonon modes couple with the exciton are taken into account. We find that the exciton Bohr radius is enlarged markedly due to these coupling. Moreover, it can be changed on a large scale by modulating the polarizability of polar substrate and the internal distance between the monolayer TMDCs and polar substrate. Theoretical result provides a potential explanation for the variation of the exciton Bohr radius in experimental measurement.

  2. Exciton-related nonlinear optical response and photoluminescence in dilute nitrogen InxGa1−xNyAs1−y/GaAs cylindrically shaped quantum dots

    International Nuclear Information System (INIS)

    Duque, C.M.; Morales, A.L.; Mora-Ramos, M.E.; Duque, C.A.

    2014-01-01

    An investigation of the effects of the dilute nitrogen contents in the exciton states of cylindrical In x Ga 1−x N y As 1−y /GaAs quantum dots is presented. The exciton states in the system are obtained within the effective mass theory and the band anti-crossing model. Exciton-related nonlinear optical absorption and refractive index change, as well as excitonic photoluminescence are studied with the help of the calculated exciton states. - Highlights: • Theoretical study of excitons in cylindrical In x Ga 1−x N y As 1−y /GaAs quantum dots. • Calculations of binding energy for different configurations of electron-hole pairs. • Nonlinear optical absorption and refractive index changes. • Dependence of photoluminescence energy transitions with several inputs

  3. Communication: Strong excitonic and vibronic effects determine the optical properties of Li₂O₂

    DEFF Research Database (Denmark)

    García Lastra, Juan Maria; Bass, J. D.; Thygesen, Kristian Sommer

    2011-01-01

    The band structure and optical absorption spectrum of lithium peroxide (Li2O2) is calculated from first-principles using the G0W0 approximation and the Bethe-Salpeter equation, respectively. A strongly localized (Frenkel type) exciton corresponding to the π*→σ* transition on the O2 −2 peroxide ion...

  4. Spectral signatures of x((5)) processes in four-wave mixing of homogeneously broadened excitons

    DEFF Research Database (Denmark)

    Langbein, W.; Meier, T.; Koch, S.W.

    2001-01-01

    -biexciton beating at the exciton resonance is observed that is vanishing for long negative delays owing to the faster dephasing in the two-exciton continuum compared with the bound biexciton state. These results are in qualitative agreement with microscopic model calculations that include the coherent dynamics...... of one- and two-exciton resonances up to the fifth order in the optical field....

  5. Near-Band-Edge Optical Responses of CH3NH3PbCl3 Single Crystals: Photon Recycling of Excitonic Luminescence

    Science.gov (United States)

    Yamada, Takumi; Aharen, Tomoko; Kanemitsu, Yoshihiko

    2018-02-01

    The determination of the band gap and exciton energies of lead halide perovskites is very important from the viewpoint of fundamental physics and photonic device applications. By using photoluminescence excitation (PLE) spectra, we reveal the optical properties of CH3NH3PbCl3 single crystals in the near-band-edge energy regime. The one-photon PLE spectrum exhibits the 1 s exciton peak at 3.11 eV. On the contrary, the two-photon PLE spectrum exhibits no peak structure. This indicates photon recycling of excitonic luminescence. By analyzing the spatial distribution of the excitons and photon recycling, we obtain 3.15 eV for the band gap energy and 41 meV for the exciton binding energy.

  6. Analytical models of optical response in one-dimensional semiconductors

    International Nuclear Information System (INIS)

    Pedersen, Thomas Garm

    2015-01-01

    The quantum mechanical description of the optical properties of crystalline materials typically requires extensive numerical computation. Including excitonic and non-perturbative field effects adds to the complexity. In one dimension, however, the analysis simplifies and optical spectra can be computed exactly. In this paper, we apply the Wannier exciton formalism to derive analytical expressions for the optical response in four cases of increasing complexity. Thus, we start from free carriers and, in turn, switch on electrostatic fields and electron–hole attraction and, finally, analyze the combined influence of these effects. In addition, the optical response of impurity-localized excitons is discussed. - Highlights: • Optical response of one-dimensional semiconductors including excitons. • Analytical model of excitonic Franz–Keldysh effect. • Computation of optical response of impurity-localized excitons

  7. Spatially indirect excitons in coupled quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Lai, Chih-Wei Eddy [Univ. of California, Berkeley, CA (United States)

    2004-03-01

    observed. The spatial and energy distributions of optically active excitons were used as thermodynamic quantities to construct a phase diagram of the exciton system, demonstrating the existence of distinct phases. Optical and electrical properties of the CQW sample were examined thoroughly to provide deeper understanding of the formation mechanisms of these cold exciton systems. These insights offer new strategies for producing cold exciton systems, which may lead to opportunities for the realization of BEC in solid-state systems.

  8. Fine structure of the exciton electroabsorption in semiconductor superlattices

    Energy Technology Data Exchange (ETDEWEB)

    Monozon, B.S., E-mail: borismonozon@mail.ru [Physics Department, Marine Technical University, 3 Lotsmanskaya Str., 190008 St.Petersburg (Russian Federation); Schmelcher, P. [Zentrum für Optische Quantentechnologien, The Hamburg Centre for Ultrafast Imaging, Universität Hamburg, Luruper Chaussee 149, 22761 Hamburg (Germany)

    2017-02-15

    Wannier-Mott excitons in a semiconductor layered superlattice (SL) are investigated analytically for the case that the period of the superlattice is much smaller than the 2D exciton Bohr radius. Additionally we assume the presence of a longitudinal external static electric field directed parallel to the SL axis. The exciton states and the optical absorption coefficient are derived in the tight-binding and adiabatic approximations. Strong and weak electric fields providing spatially localized and extended electron and hole states, respectively, are studied. The dependencies of the exciton states and the exciton absorption spectrum on the SL parameters and the electric field strength are presented in an explicit form. We focus on the fine structure of the ground quasi-2D exciton level formed by the series of closely spaced energy levels adjacent from the high frequencies. These levels are related to the adiabatically slow relative exciton longitudinal motion governed by the potential formed by the in-plane exciton state. It is shown that the external electric fields compress the fine structure energy levels, decrease the intensities of the corresponding optical peaks and increase the exciton binding energy. A possible experimental study of the fine structure of the exciton electroabsorption is discussed.

  9. Synthetic Control of Exciton Behavior in Colloidal Quantum Dots.

    Science.gov (United States)

    Pu, Chaodan; Qin, Haiyan; Gao, Yuan; Zhou, Jianhai; Wang, Peng; Peng, Xiaogang

    2017-03-08

    Colloidal quantum dots are promising optical and optoelectronic materials for various applications, whose performance is dominated by their excited-state properties. This article illustrates synthetic control of their excited states. Description of the excited states of quantum-dot emitters can be centered around exciton. We shall discuss that, different from conventional molecular emitters, ground-state structures of quantum dots are not necessarily correlated with their excited states. Synthetic control of exciton behavior heavily relies on convenient and affordable monitoring tools. For synthetic development of ideal optical and optoelectronic emitters, the key process is decay of band-edge excitons, which renders transient photoluminescence as important monitoring tool. On the basis of extensive synthetic developments in the past 20-30 years, synthetic control of exciton behavior implies surface engineering of quantum dots, including surface cation/anion stoichiometry, organic ligands, inorganic epitaxial shells, etc. For phosphors based on quantum dots doped with transition metal ions, concentration and location of the dopant ions within a nanocrystal lattice are found to be as important as control of the surface states in order to obtain bright dopant emission with monoexponential yet tunable photoluminescence decay dynamics.

  10. Exciton Binding Energy of Monolayer WS2

    Science.gov (United States)

    Zhu, Bairen; Chen, Xi; Cui, Xiaodong

    2015-03-01

    The optical properties of monolayer transition metal dichalcogenides (TMDC) feature prominent excitonic natures. Here we report an experimental approach to measuring the exciton binding energy of monolayer WS2 with linear differential transmission spectroscopy and two-photon photoluminescence excitation spectroscopy (TP-PLE). TP-PLE measurements show the exciton binding energy of 0.71 +/- 0.01 eV around K valley in the Brillouin zone.

  11. Optical absorptions of an exciton in a quantum ring: Effect of the repulsive core

    International Nuclear Information System (INIS)

    Xie, Wenfang

    2013-01-01

    We study the optical absorptions of an exciton in a quantum ring. The quantum ring is described as a circular quantum dot with a repulsive core. The advantage of our methodology is that one can investigate the influence of the repulsive core by varying two parameters in the confinement potential. The linear, third-order nonlinear and total optical absorption coefficients have been examined with the change of the confinement potential. The results show that the optical absorptions are strongly affected by the repulsive core. Moreover, the repulsive core can influence the oscillation in the resonant peak of the absorption coefficients.

  12. Direct observation of free-exciton thermalization in quantum-well structures

    DEFF Research Database (Denmark)

    Umlauff, M.; Hoffmann, J.; Kalt, H.

    1998-01-01

    We report on a direct observation of free-exciton thermalization in quantum-well structures. A narrow energy distribution of free 1s excitons is created in ZnSe-based quantum wells by emission of one LO phonon after optical excitation of the continuum stales with picosecond laser pulses. The subs......We report on a direct observation of free-exciton thermalization in quantum-well structures. A narrow energy distribution of free 1s excitons is created in ZnSe-based quantum wells by emission of one LO phonon after optical excitation of the continuum stales with picosecond laser pulses...

  13. Coherent quantum dynamics of excitons in monolayer transition metal dichalcogenides

    KAUST Repository

    Moody, Galan

    2016-03-14

    Transition metal dichalcogenides (TMDs) have garnered considerable interest in recent years owing to their layer thickness-dependent optoelectronic properties. In monolayer TMDs, the large carrier effective masses, strong quantum confinement, and reduced dielectric screening lead to pronounced exciton resonances with remarkably large binding energies and coupled spin and valley degrees of freedom (valley excitons). Coherent control of valley excitons for atomically thin optoelectronics and valleytronics requires understanding and quantifying sources of exciton decoherence. In this work, we reveal how exciton-exciton and exciton-phonon scattering influence the coherent quantum dynamics of valley excitons in monolayer TMDs, specifically tungsten diselenide (WSe2), using two-dimensional coherent spectroscopy. Excitation-density and temperature dependent measurements of the homogeneous linewidth (inversely proportional to the optical coherence time) reveal that exciton-exciton and exciton-phonon interactions are significantly stronger compared to quasi-2D quantum wells and 3D bulk materials. The residual homogeneous linewidth extrapolated to zero excitation density and temperature is ~1:6 meV (equivalent to a coherence time of 0.4 ps), which is limited only by the population recombination lifetime in this sample. © (2016) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.

  14. Coherent quantum dynamics of excitons in monolayer transition metal dichalcogenides

    KAUST Repository

    Moody, Galan; Hao, Kai; Dass, Chandriker Kavir; Singh, Akshay; Xu, Lixiang; Tran, Kha; Chen, Chang-Hsiao; Li, Ming-yang; Li, Lain-Jong; Clark, Genevieve; Bergh ä user, Gunnar; Malic, Ermin; Knorr, Andreas; Xu, Xiaodong; Li, Xiaoqin

    2016-01-01

    Transition metal dichalcogenides (TMDs) have garnered considerable interest in recent years owing to their layer thickness-dependent optoelectronic properties. In monolayer TMDs, the large carrier effective masses, strong quantum confinement, and reduced dielectric screening lead to pronounced exciton resonances with remarkably large binding energies and coupled spin and valley degrees of freedom (valley excitons). Coherent control of valley excitons for atomically thin optoelectronics and valleytronics requires understanding and quantifying sources of exciton decoherence. In this work, we reveal how exciton-exciton and exciton-phonon scattering influence the coherent quantum dynamics of valley excitons in monolayer TMDs, specifically tungsten diselenide (WSe2), using two-dimensional coherent spectroscopy. Excitation-density and temperature dependent measurements of the homogeneous linewidth (inversely proportional to the optical coherence time) reveal that exciton-exciton and exciton-phonon interactions are significantly stronger compared to quasi-2D quantum wells and 3D bulk materials. The residual homogeneous linewidth extrapolated to zero excitation density and temperature is ~1:6 meV (equivalent to a coherence time of 0.4 ps), which is limited only by the population recombination lifetime in this sample. © (2016) COPYRIGHT Society of Photo-Optical Instrumentation Engineers (SPIE). Downloading of the abstract is permitted for personal use only.

  15. Excitons in van der Waals Heterostructures: A theoretical study

    DEFF Research Database (Denmark)

    Latini, Simone

    )electronics devices, e.g. light emitting diodes, solar cells, ultra-fast photodetectors, transistors etc., have been successfully fabricated. It is well established that for isolated 2D semiconductors and vdWHs the optical response is governed by excitonic effects. While it is understood that the reduced amount...... of electronic screening in freestanding 2D materials is the main origin of extraordinarily strongly bound excitons, a theoretical understanding of excitonic effects and of how the electronic screening is affected for the more complex case of multi-layer structures is still lacking due to the computational...... in a generalized hydrogenic model to compute exciton binding energies in isolated, supported, or encapsulated 2D semiconductors. The non-locality of the dielectric screening is inherently included in our method and we can successfully describe the non-hydrogenic Rydberg series of low-dimensional systems...

  16. Exciton-related nonlinear optical absorption and refractive index change in GaAs-Ga{sub 1-x}Al{sub x}As double quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Miranda, Guillermo L. [Fisica Teorica y Aplicada, Escuela de Ingenieria de Antioquia, A.A. 7516 Medellin (Colombia); Instituto de Fisica, Universidad de Antioquia, AA 1226 Medellin (Colombia); Mora-Ramos, Miguel E., E-mail: memora@uaem.mx [Fisica Teorica y Aplicada, Escuela de Ingenieria de Antioquia, A.A. 7516 Medellin (Colombia); Facultad de Ciencias, Universidad Autonoma del Estado de Morelos, Av. Universidad 1001, C.P. 62209 Cuernavaca, Morelos (Mexico); Instituto de Fisica, Universidad de Antioquia, AA 1226 Medellin (Colombia); Duque, Carlos A. [Instituto de Fisica, Universidad de Antioquia, AA 1226 Medellin (Colombia)

    2013-01-15

    In this work the variations of the exciton-related optical absorption and the change of the refractive index in a GaAs-(Ga,Al)As double quantum well as functions of the geometric parameters of the heterostructure are investigated. The variational method is applied within the framework of the parabolic band and effective mass approximations, in order to obtain the 1s-like exciton energy spectrum. The outcome for the related optical coefficients shows a quenched and redshifted light absorption as a result of the increment in the inner barrier and right-hand well widths, with the possibility of an enhancement of the excitonic contribution to the relative change in the refractive index.

  17. Magneto-exciton dephasing in a single quantum dot

    Science.gov (United States)

    Rodriguez, F. J.; Reyes, A.; Olaya-Castro, A.; Quiroga, L.

    2001-03-01

    Ultrafast spectroscopy experiments on single quantum dot (SQD) in magnetic fields provide a variety of unexpected results, one of them being the recently reported entanglement of exciton states. In order to explore the entanglement robustness, dephasing mechanisms must be considered. By calculating the non-linear time resolved optical spectrum of a SQD, we present a theoretical study on the exciton-exciton scattering contribution to the magneto-exciton dephasing time. Our results show that the time evolution of \\chi^(3) presents, under non-steady-state condition, a beating between the bound biexciton and the first unbound biexciton state in the strong confinement regime. The contribution coming from both left and right polarized emitted photons allows us to predict the creation of exciton entanglement, in agreement with recent experimental results. Previous theoretical works have only addressed the stationary optical response. By contrast, our results based on a full time dependent calculation show new features specially for the fast dephasing case.

  18. Interlayer excitons in a bulk van der Waals semiconductor

    DEFF Research Database (Denmark)

    Arora, Ashish; Drueppel, Matthias; Schmidt, Robert

    2017-01-01

    Bound electron-hole pairs called excitons govern the electronic and optical response of many organic and inorganic semiconductors. Excitons with spatially displaced wave functions of electrons and holes (interlayer excitons) are important for Bose-Einstein condensation, superfluidity......, dissipationless current flow, and the light-induced exciton spin Hall effect. Here we report on the discovery of interlayer excitons in a bulk van der Waals semiconductor. They form due to strong localization and spin-valley coupling of charge carriers. By combining high-field magneto-reflectance experiments...

  19. Skyrmion formation and optical spin-Hall effect in an expanding coherent cloud of indirect excitons.

    Science.gov (United States)

    Vishnevsky, D V; Flayac, H; Nalitov, A V; Solnyshkov, D D; Gippius, N A; Malpuech, G

    2013-06-14

    We provide a theoretical description of the polarization pattern and phase singularities experimentally evidenced recently in a condensate of indirect excitons [H. High et al., Nature 483, 584 (2012)]. We show that the averaging of the electron and hole orbital motion leads to a comparable spin-orbit interaction for both types of carriers. We demonstrate that the interplay between a radial coherent flux of bright indirect excitons and the Dresselhaus spin-orbit interaction results in the formation of spin domains and of topological defects similar to Skyrmions. We reproduce qualitatively all the features of the experimental data and obtain a polarization pattern as in the optical spin-Hall effect despite the different symmetry of the spin-orbit interactions.

  20. Decay of orientational grating of weakly confined excitons in GaAs thin films

    International Nuclear Information System (INIS)

    Kojima, O.; Isu, T.; Ishi-Hayase, J.; Kanno, A.; Katouf, R.; Sasaki, M.; Tsuchiya, M.

    2008-01-01

    We report the dynamical properties of the exciton orientation in GaAs thin films using the orientational grating (OG) technique. From the results of excitation-power dependence of OG signal, we confirmed that the OG signal comes from the optical nonlinearity of weakly confined excitons. In addition, the OG-decay time decreases with an increase of excitation power due to exciton-exciton interaction, and the shortest decay time is below 1 ps. Our results may imply the potential application of optical nonlinearity of weakly confined exciton to ultrafast switching devices operating at 1 Tbit/s

  1. Coherent detection of THz-induced sideband emission from excitons in the nonperturbative regime

    Science.gov (United States)

    Uchida, K.; Otobe, T.; Mochizuki, T.; Kim, C.; Yoshita, M.; Tanaka, K.; Akiyama, H.; Pfeiffer, L. N.; West, K. W.; Hirori, H.

    2018-04-01

    Strong interaction of a terahertz (THz) wave with excitons induces nonperturbative optical effects such as Rabi splitting and high-order sideband generation. Here, we investigated coherent properties of THz-induced sideband emissions from GaAs/AlGaAs multiquantum wells. With increasing THz electric field, optical susceptibility of the THz-dressed exciton shows a redshift with spectral broadening and extraordinary phase shift. This implies that the field ionization of the 1 s exciton modifies the THz-dressed exciton in the nonperturbative regime.

  2. NONLINEAR OPTICAL PHENOMENA: Self-reflection in a system of excitons and biexcitons in semiconductors

    Science.gov (United States)

    Khadzhi, P. I.; Lyakhomskaya, K. D.

    1999-10-01

    The characteristic features of the self-reflection of a powerful electromagnetic wave in a system of coherent excitons and biexcitons in semiconductors were investigated as one of the manifestations of the nonlinear optical skin effect. It was found that a monotonically decreasing standing wave with an exponentially falling spatial tail is formed in the surface region of a semiconductor. Under the influence of the field of a powerful pulse, an optically homogeneous medium is converted into one with distributed feedback. The appearance of spatially separated narrow peaks of the refractive index, extinction coefficient, and reflection coefficient is predicted.

  3. Elastic strain engineering of quantum dot excitonic emission in nanomembranes and optical resonators

    Energy Technology Data Exchange (ETDEWEB)

    Ding, Fei; Plumhof, Johannes; Rastelli, Armando; Schmidt, Oliver [Institute for Integrative Nanosciences, IFW Dresden (Germany); Singh, Ranber; Zander, Tim; Bester, Gabriel [Max-Planck-Institut fuer Festkoerperforschung, Stuttgart (Germany)

    2010-07-01

    We study the effect of an external biaxial stress on the light emission of single InGaAs/GaAs(001) quantum dots (QD) embedded in a 200 nm-thick-membrane. Reversible and bi-directional spectral tuning of QD excitonic emission is demonstrated via a simple electro-mechanical device. The most intriguing finding is that biaxial strain is a reliable tool to engineer the QD electronic structure and reach color coincidence between exciton and biexciton emission, providing a vital prerequisite for the generation of polarization entangled photon pairs through a time reordering strategy. The physical origin of this new phenomenon is discussed based on the empirical pseudopotential calculations. With similar technique we study the effect of biaxial stress on single QDs embedded in microring resonators. The microrings can be reversibly stretched or squeezed, resulting in a controllable engineering of both QD emissions and optical modes. Our results open up a new tuning strategy to study cQED with semiconductor quantum dots.

  4. Modeling temperature dependent singlet exciton dynamics in multilayered organic nanofibers

    Science.gov (United States)

    de Sousa, Leonardo Evaristo; de Oliveira Neto, Pedro Henrique; Kjelstrup-Hansen, Jakob; da Silva Filho, Demétrio Antônio

    2018-05-01

    Organic nanofibers have shown potential for application in optoelectronic devices because of the tunability of their optical properties. These properties are influenced by the electronic structure of the molecules that compose the nanofibers and also by the behavior of the excitons generated in the material. Exciton diffusion by means of Förster resonance energy transfer is responsible, for instance, for the change with temperature of colors in the light emitted by systems composed of different types of nanofibers. To study in detail this mechanism, we model temperature dependent singlet exciton dynamics in multilayered organic nanofibers. By simulating absorption and emission spectra, the possible Förster transitions are identified. Then, a kinetic Monte Carlo model is employed in combination with a genetic algorithm to theoretically reproduce time-resolved photoluminescence measurements for several temperatures. This procedure allows for the obtainment of different information regarding exciton diffusion in such a system, including temperature effects on the Förster transfer efficiency and the activation energy of the Förster mechanism. The method is general and may be employed for different systems where exciton diffusion plays a role.

  5. Excitonic processes at organic heterojunctions

    Science.gov (United States)

    He, ShouJie; Lu, ZhengHong

    2018-02-01

    Understanding excitonic processes at organic heterojunctions is crucial for development of organic semiconductor devices. This article reviews recent research on excitonic physics that involve intermolecular charge transfer (CT) excitons, and progress on understanding relationships between various interface energy levels and key parameters governing various competing interface excitonic processes. These interface excitonic processes include radiative exciplex emission, nonradiative recombination, Auger electron emission, and CT exciton dissociation. This article also reviews various device applications involving interface CT excitons, such as organic light-emitting diodes (OLEDs), organic photovoltaic cells, organic rectifying diodes, and ultralow-voltage Auger OLEDs.

  6. Decoherence processes during optical manipulation of excitonic qubits in semiconductor quantum dots

    Science.gov (United States)

    Wang, Q. Q.; Muller, A.; Bianucci, P.; Rossi, E.; Xue, Q. K.; Takagahara, T.; Piermarocchi, C.; MacDonald, A. H.; Shih, C. K.

    2005-07-01

    Using photoluminescence spectroscopy, we have investigated the nature of Rabi oscillation damping during optical manipulation of excitonic qubits in self-assembled quantum dots. Rabi oscillations were recorded by varying the pulse amplitude for fixed pulse durations between 4ps and 10ps . Up to five periods are visible, making it possible to quantify the excitation dependent damping. We find that this damping is more pronounced for shorter pulse widths and show that its origin is the nonresonant excitation of carriers in the wetting layer, most likely involving bound-to-continuum and continuum-to-bound transitions.

  7. Exciton-related nonlinear optical response and photoluminescence in dilute nitrogen In{sub x}Ga{sub 1−x}N{sub y}As{sub 1−y}/GaAs cylindrically shaped quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Duque, C.M.; Morales, A.L. [Grupo de Materia Condensada-UdeA, Instituto de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín (Colombia); Mora-Ramos, M.E. [Grupo de Materia Condensada-UdeA, Instituto de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín (Colombia); Facultad de Ciencias, Universidad Autónoma del Estado de Morelos, Av. Universidad 1001, CP 62209 Cuernavaca, Morelos (Mexico); Duque, C.A. [Grupo de Materia Condensada-UdeA, Instituto de Física, Facultad de Ciencias Exactas y Naturales, Universidad de Antioquia UdeA, Calle 70 No. 52-21, Medellín (Colombia)

    2014-10-15

    An investigation of the effects of the dilute nitrogen contents in the exciton states of cylindrical In{sub x}Ga{sub 1−x}N{sub y}As{sub 1−y}/GaAs quantum dots is presented. The exciton states in the system are obtained within the effective mass theory and the band anti-crossing model. Exciton-related nonlinear optical absorption and refractive index change, as well as excitonic photoluminescence are studied with the help of the calculated exciton states. - Highlights: • Theoretical study of excitons in cylindrical In{sub x}Ga{sub 1−x}N{sub y}As{sub 1−y}/GaAs quantum dots. • Calculations of binding energy for different configurations of electron-hole pairs. • Nonlinear optical absorption and refractive index changes. • Dependence of photoluminescence energy transitions with several inputs.

  8. Optical orientation of the homogeneous non-equilibrium Bose-Einstein condensate of bright excitons (polaritons)

    OpenAIRE

    Korenev, V. L.

    2011-01-01

    A simple model, describing the dynamics of the non-equilibrium pseudospin of a homogeneous Bose-Einstein condensate of exciton polaritons, has been formulated. It explains the suppression of spin splitting of a non-equilibrium polariton condensate in an external magnetic field, the optical alignment, and the conversion of alignment into orientation of polaritons. It has been shown that inverse effects are possible, to wit, the spontaneous circular polarization and the enhancement of spin spli...

  9. Influence of the sign of the coupling on the temperature dependence of optical properties of one-dimensional exciton models

    Energy Technology Data Exchange (ETDEWEB)

    Cruzeiro, L [CCMAR and FCT, Universidade of Algarve, Campus de Gambelas, 8005-139 Faro (Portugal)

    2008-10-14

    A new physical cause for a temperature-dependent double peak in exciton systems is put forward within a thermal equilibrium approach for the calculation of optical properties of exciton systems. Indeed, it is found that one-dimensional exciton systems with only one molecule per unit cell can have an absorption spectrum characterized by a double peak provided that the coupling between excitations in different molecules is positive. The two peaks, whose relative intensities vary with temperature, are located around the exciton band edges, being separated by an energy of approximately 4V, where V is the average coupling between nearest neighbours. For small amounts of diagonal and off-diagonal disorder, the contributions from the intermediate states in the band are also visible as intermediate structure between the two peaks, this being enhanced for systems with periodic boundary conditions. At a qualitative level, these results correlate well with experimental observations in the molecular aggregates of the thiacarbocyanine dye THIATS and in the organic crystals of acetanilide and N-methylacetamide.

  10. Influence of the sign of the coupling on the temperature dependence of optical properties of one-dimensional exciton models

    International Nuclear Information System (INIS)

    Cruzeiro, L

    2008-01-01

    A new physical cause for a temperature-dependent double peak in exciton systems is put forward within a thermal equilibrium approach for the calculation of optical properties of exciton systems. Indeed, it is found that one-dimensional exciton systems with only one molecule per unit cell can have an absorption spectrum characterized by a double peak provided that the coupling between excitations in different molecules is positive. The two peaks, whose relative intensities vary with temperature, are located around the exciton band edges, being separated by an energy of approximately 4V, where V is the average coupling between nearest neighbours. For small amounts of diagonal and off-diagonal disorder, the contributions from the intermediate states in the band are also visible as intermediate structure between the two peaks, this being enhanced for systems with periodic boundary conditions. At a qualitative level, these results correlate well with experimental observations in the molecular aggregates of the thiacarbocyanine dye THIATS and in the organic crystals of acetanilide and N-methylacetamide

  11. Exciton correlations and input–output relations in non-equilibrium exciton superfluids

    International Nuclear Information System (INIS)

    Ye, Jinwu; Sun, Fadi; Yu, Yi-Xiang; Liu, Wuming

    2013-01-01

    The photoluminescence (PL) measurements on photons and the transport measurements on excitons are the two types of independent and complementary detection tools to search for possible exciton superfluids in electron–hole semi-conductor bilayer systems. In fact, it was believed that the transport measurements can provide more direct evidences on superfluids than the spectroscopic measurements. It is important to establish the relations between the two kinds of measurements. In this paper, using quantum Heisenberg–Langevin equations, we establish such a connection by calculating various exciton correlation functions in the putative exciton superfluids. These correlation functions include both normal and anomalous greater, lesser, advanced, retarded, and time-ordered exciton Green functions and also various two exciton correlation functions. We also evaluate the corresponding normal and anomalous spectral weights and the Keldysh distribution functions. We stress the violations of the fluctuation and dissipation theorem among these various exciton correlation functions in the non-equilibrium exciton superfluids. We also explore the input–output relations between various exciton correlation functions and those of emitted photons such as the angle resolved photon power spectrum, phase sensitive two mode squeezing spectrum and two photon correlations. Applications to possible superfluids in the exciton–polariton systems are also mentioned. For a comparison, using conventional imaginary time formalism, we also calculate all the exciton correlation functions in an equilibrium dissipative exciton superfluid in the electron–electron coupled semi-conductor bilayers at the quantum Hall regime at the total filling factor ν T =1. We stress the analogies and also important differences between the correlations functions in the two exciton superfluid systems. - Highlights: ► Establish the relations between photoluminescence and transport measurements. ► Stress the

  12. Quasienergy Spectroscopy of Excitons

    DEFF Research Database (Denmark)

    Johnsen, Kristinn; Jauho, Antti-Pekka

    1999-01-01

    We theoretically study nonlinear optics of excitons under intense THz irradiation. In particular, the linear near-infrared absorption and resonantly enhanced nonlinear sideband generation are described. We predict a rich structure in the spectra which an be interpreted in terms of the quasienergy...

  13. Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides

    KAUST Repository

    Moody, Galan

    2015-09-18

    The band-edge optical response of transition metal dichalcogenides, an emerging class of atomically thin semiconductors, is dominated by tightly bound excitons localized at the corners of the Brillouin zone (valley excitons). A fundamental yet unknown property of valley excitons in these materials is the intrinsic homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Here we use optical two-dimensional Fourier transform spectroscopy to measure the exciton homogeneous linewidth in monolayer tungsten diselenide (WSe2). The homogeneous linewidth is found to be nearly two orders of magnitude narrower than the inhomogeneous width at low temperatures. We evaluate quantitatively the role of exciton–exciton and exciton–phonon interactions and population relaxation as linewidth broadening mechanisms. The key insights reported here—strong many-body effects and intrinsically rapid radiative recombination—are expected to be ubiquitous in atomically thin semiconductors.

  14. Halogenation of SiC for band-gap engineering and excitonic functionalization

    Science.gov (United States)

    Drissi, L. B.; Ramadan, F. Z.; Lounis, S.

    2017-11-01

    The optical excitation spectra and excitonic resonances are investigated in systematically functionalized SiC with Fluorine and/or Chlorine utilizing density functional theory in combination with many-body perturbation theory. The latter is required for a realistic description of the energy band-gaps as well as for the theoretical realization of excitons. Structural, electronic and optical properties are scrutinized and show the high stability of the predicted two-dimensional materials. Their realization in laboratory is thus possible. Large band-gaps of the order of 4 eV are found in the so-called GW approximation, with the occurrence of bright excitons, optically active in the four investigated materials. Their binding energies vary from 0.9 eV to 1.75 eV depending on the decoration choice and in one case, a dark exciton is foreseen to exist in the fully chlorinated SiC. The wide variety of opto-electronic properties suggest halogenated SiC as interesting materials with potential not only for solar cell applications, anti-reflection coatings or high-reflective systems but also for a possible realization of excitonic Bose-Einstein condensation.

  15. Excitons in the Fractional Quantum Hall Effect

    Science.gov (United States)

    Laughlin, R. B.

    1984-09-01

    Quasiparticles of charge 1/m in the Fractional Quantum Hall Effect form excitons, which are collective excitations physically similar to the transverse magnetoplasma oscillations of a Wigner crystal. A variational exciton wavefunction which shows explicitly that the magnetic length is effectively longer for quasiparticles than for electrons is proposed. This wavefunction is used to estimate the dispersion relation of these excitons and the matrix elements to generate them optically out of the ground state. These quantities are then used to describe a type of nonlinear conductivity which may occur in these systems when they are relatively clean.

  16. Biexciton formation and exciton coherent coupling in layered GaSe

    Science.gov (United States)

    Dey, P.; Paul, J.; Moody, G.; Stevens, C. E.; Glikin, N.; Kovalyuk, Z. D.; Kudrynskyi, Z. R.; Romero, A. H.; Cantarero, A.; Hilton, D. J.; Karaiskaj, D.

    2015-06-01

    Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ˜2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with "ab initio" theoretical calculations of the phonon spectra, indicate strong interaction with the A1 ' phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal.

  17. Tailoring Quantum Dot Assemblies to Extend Exciton Coherence Times and Improve Exciton Transport

    Science.gov (United States)

    Seward, Kenton; Lin, Zhibin; Lusk, Mark

    2012-02-01

    The motion of excitons through nanostructured assemblies plays a central role in a wide range of physical phenomena including quantum computing, molecular electronics, photosynthetic processes, excitonic transistors and light emitting diodes. All of these technologies are severely handicapped, though, by quasi-particle lifetimes on the order of a nanosecond. The movement of excitons must therefore be as efficient as possible in order to move excitons meaningful distances. This is problematic for assemblies of small Si quantum dots (QDs), where excitons quickly localize and entangle with dot phonon modes. Ensuing exciton transport is then characterized by a classical random walk reduced to very short distances because of efficient recombination. We use a combination of master equation (Haken-Strobl) formalism and density functional theory to estimate the rate of decoherence in Si QD assemblies and its impact on exciton mobility. Exciton-phonon coupling and Coulomb interactions are calculated as a function of dot size, spacing and termination to minimize the rate of intra-dot phonon entanglement. This extends the time over which more efficient exciton transport, characterized by partial coherence, can be maintained.

  18. Excitons in Core-Shell Nanowires with Polygonal Cross Sections.

    Science.gov (United States)

    Sitek, Anna; Urbaneja Torres, Miguel; Torfason, Kristinn; Gudmundsson, Vidar; Bertoni, Andrea; Manolescu, Andrei

    2018-04-11

    The distinctive prismatic geometry of semiconductor core-shell nanowires leads to complex localization patterns of carriers. Here, we describe the formation of optically active in-gap excitonic states induced by the interplay between localization of carriers in the corners and their mutual Coulomb interaction. To compute the energy spectra and configurations of excitons created in the conductive shell, we use a multielectron numerical approach based on the exact solution of the multiparticle Hamiltonian for electrons in the valence and conduction bands, which includes the Coulomb interaction in a nonperturbative manner. We expose the formation of well-separated quasidegenerate levels, and focus on the implications of the electron localization in the corners or on the sides of triangular, square, and hexagonal cross sections. We obtain excitonic in-gap states associated with symmetrically distributed electrons in the spin singlet configuration. They acquire large contributions due to Coulomb interaction, and thus are shifted to much higher energies than other states corresponding to the conduction electron and the vacancy localized in the same corner. We compare the results of the multielectron method with those of an electron-hole model, and we show that the latter does not reproduce the singlet excitonic states. We also obtain the exciton lifetime and explain selection rules which govern the recombination process.

  19. Probing long-lived dark excitons in self-assembled quantum dots

    DEFF Research Database (Denmark)

    Johansen, Jeppe; Julsgaard, Brian; Stobbe, Søren

    2010-01-01

    Long-lived dark exciton states are formed in self-assembled quantum dots due to the combination of the angular momentum of electrons and holes. The lifetime of dark excitons are determined by spin-flip processes that transfer dark excitons into radiative bright excitons. We employ time......-resolved spontaneous emission measurements in a modified local density of optical states to unambiguously record the spin-flip rate. Pronounced variations in the spin-flip rate with the quantum dot emission energy are observed demonstrating that the exciton storage time can be extended by controlling the quantum dot......, which illustrates the important role of interfaces for quantum dot based nanophotonic structures....

  20. Exciton Rydberg series in mono- and few-layer WS2

    Science.gov (United States)

    Chernikov, Alexey; Berkelbach, Timothy C.; Hill, Heather M.; Rigosi, Albert; Li, Yilei; Aslan, Özgur B.; Hybertsen, Mark S.; Reichman, David R.; Heinz, Tony F.

    2014-03-01

    Considered a long-awaited semiconducting analogue to graphene, the family of atomically thin transition metal dichalcogenides (TMDs) attracted intense interest in the scientific community due to their remarkable physical properties resulting from the reduced dimensionality. A fundamental manifestation of the two-dimensional nature is a strong increase in the Coulomb interaction. The resulting formation of tightly bound excitons plays a crucial role for a majority of optical and transport phenomena. In our work, we investigate the excitons in atomically thin TMDs by optical micro-spectroscopy and apply a microscopic, ab-initio theoretical approach. We observe a full sequence of excited exciton states, i.e., the Rydberg series, in the monolayer WS2, identifying tightly bound excitons with energies exceeding 0.3 eV - almost an order of magnitude higher than in the corresponding, three-dimensional crystal. We also find significant deviations of the excitonic properties from the conventional hydrogenic physics - a direct evidence of a non-uniform dielectric environment. Finally, an excellent quantitative agreement is obtained between the experimental findings and the developed theoretical approach.

  1. Observation of surface excitons in rare gas solids

    International Nuclear Information System (INIS)

    Saile, V.; Skibowski, M.; Steinmann, W.; Guertler, P.; Koch, E.E.; Kozevnikov, A.

    1976-04-01

    Evidence is obtained for the excitation of surface excitons in solid Ar, Kr and Xe in optical transmission and reflection experiments using synchrotron radiation. They are located at photon energies ranging from 0.6 eV for Ar to 0.1 eV for Xe below the corresponding bulk excitons excited from the valence bands. Their halfwidths (20-50 MeV) is less than half the values found for the bulk excitons. Some are split by an amount considerably smaller than the spin orbit splitting of the valence bands. (orig.) [de

  2. Singlet Exciton Lifetimes in Conjugated Polymer Films for Organic Solar Cells

    KAUST Repository

    Dimitrov, Stoichko

    2016-01-13

    The lifetime of singlet excitons in conjugated polymer films is a key factor taken into account during organic solar cell device optimization. It determines the singlet exciton diffusion lengths in polymer films and has a direct impact on the photocurrent generation by organic solar cell devices. However, very little is known about the material properties controlling the lifetimes of singlet excitons, with most of our knowledge originating from studies of small organic molecules. Herein, we provide a brief summary of the nature of the excited states in conjugated polymer films and then present an analysis of the singlet exciton lifetimes of 16 semiconducting polymers. The exciton lifetimes of seven of the studied polymers were measured using ultrafast transient absorption spectroscopy and compared to the lifetimes of seven of the most common photoactive polymers found in the literature. A plot of the logarithm of the rate of exciton decay vs. the polymer optical bandgap reveals a medium correlation between lifetime and bandgap, thus suggesting that the Energy Gap Law may be valid for these systems. This therefore suggests that small bandgap polymers can suffer from short exciton lifetimes, which may limit their performance in organic solar cell devices. In addition, the impact of film crystallinity on the exciton lifetime was assessed for a small bandgap diketopyrrolopyrrole co-polymer. It is observed that the increase of polymer film crystallinity leads to reduction in exciton lifetime and optical bandgap again in agreement with the Energy Gap Law.

  3. Bose-Einstein condensation and indirect excitons: a review.

    Science.gov (United States)

    Combescot, Monique; Combescot, Roland; Dubin, François

    2017-06-01

    We review recent progress on Bose-Einstein condensation (BEC) of semiconductor excitons. The first part deals with theory, the second part with experiments. This Review is written at a time where the problem of exciton Bose-Einstein condensation has just been revived by the understanding that the exciton condensate must be dark because the exciton ground state is not coupled to light. Here, we theoretically discuss this missed understanding before providing its experimental support through experiments that scrutinize indirect excitons made of spatially separated electrons and holes. The theoretical part first discusses condensation of elementary bosons. In particular, the necessary inhibition of condensate fragmentation by exchange interaction is stressed, before extending the discussion to interacting bosons with spin degrees of freedom. The theoretical part then considers composite bosons made of two fermions like semiconductor excitons. The spin structure of the excitons is detailed, with emphasis on the crucial fact that ground-state excitons are dark: indeed, this imposes the exciton Bose-Einstein condensate to be not coupled to light in the dilute regime. Condensate fragmentations are then reconsidered. In particular, it is shown that while at low density, the exciton condensate is fully dark, it acquires a bright component, coherent with the dark one, beyond a density threshold: in this regime, the exciton condensate is 'gray'. The experimental part first discusses optical creation of indirect excitons in quantum wells, and the detection of their photoluminescence. Exciton thermalisation is also addressed, as well as available approaches to estimate the exciton density. We then switch to specific experiments where indirect excitons form a macroscopic fragmented ring. We show that such ring provides efficient electrostatic trapping in the region of the fragments where an essentially-dark exciton Bose-Einstein condensate is formed at sub-Kelvin bath

  4. Excitonic bistabilities, instabilities and chaos in laser-pumped semiconductor

    International Nuclear Information System (INIS)

    Nguyen Ba An; Nguyen Trung Dan; Hoang Xuan Nguyen

    1992-07-01

    The Hurwitz criteria are used for a stability analysis of the steady state excitonic optical bistability curves in a semiconductor pumped by an external laser resonant with the exciton level. Besides the middle branch of the bistability curves which is unstable in the sense of the linear stability theory, we have found other domains of instability in the upper and lower branches of the steady state curves. Numerical results show that a possible route to chaos in the photon-exciton system is period-doubling self-oscillation process. The influence of the presence of free carriers that coexist with the excitons is also discussed. (author). 16 refs, 6 figs

  5. Coulomb Mediated Hybridization of Excitons in Coupled Quantum Dots.

    Science.gov (United States)

    Ardelt, P-L; Gawarecki, K; Müller, K; Waeber, A M; Bechtold, A; Oberhofer, K; Daniels, J M; Klotz, F; Bichler, M; Kuhn, T; Krenner, H J; Machnikowski, P; Finley, J J

    2016-02-19

    We report Coulomb mediated hybridization of excitonic states in optically active InGaAs quantum dot molecules. By probing the optical response of an individual quantum dot molecule as a function of the static electric field applied along the molecular axis, we observe unexpected avoided level crossings that do not arise from the dominant single-particle tunnel coupling. We identify a new few-particle coupling mechanism stemming from Coulomb interactions between different neutral exciton states. Such Coulomb resonances hybridize the exciton wave function over four different electron and hole single-particle orbitals. Comparisons of experimental observations with microscopic eight-band k·p calculations taking into account a realistic quantum dot geometry show good agreement and reveal that the Coulomb resonances arise from broken symmetry in the artificial semiconductor molecule.

  6. Spectroscopy and photophysics of self-organized zinc porphyrin nanolayers. 1. Optical spectroscopy of excitonic interactions involving the soret band

    NARCIS (Netherlands)

    Donker, H.; Koehorst, R.B.M.; Schaafsma, T.J.

    2005-01-01

    The photophysical properties of excited singlet states of zinc tetra-(p-octylphenyl)-porphyrin in 5-25-nm-thick films spin-coated onto quartz slides have been investigated by optical spectroscopy. Analysis of the polarized absorption spectra using a dipole-dipole exciton model with two mutually

  7. Exciton center-of-mass localization and dielectric environment effect in monolayer WS2

    Science.gov (United States)

    Hichri, Aïda; Ben Amara, Imen; Ayari, Sabrine; Jaziri, Sihem

    2017-06-01

    The ultrathin transition metal dichalcogenides (TMDs) have emerged as promising materials for various applications using two dimensional semiconductors. They have attracted increasing attention due to their unique optical properties originate from neutral and charged excitons. In this paper, we study the strong localization of exciton center-of-mass motion within random potential fluctuations caused by the monolayer defects. Here, we report negatively charged exciton formation in monolayer TMDs, notably tungsten disulfide WS2. Our theory is based on an effective mass model of neutral and charged excitons, parameterized by ab-initio calculations. Taking into the account the strong correlation between the monolayer WS2 and the surrounding dielectric environment, our theoretical results are in good agreement with one-photon photoluminescence (PL) and reflectivity measurements. We also show that the exciton state with p-symmetry, experimentally observed by two-photon PL emission, is energetically below the 2s-state. We use the equilibrium mass action law, to quantify the relative weight of exciton and trion PL. We show that exciton and trion emission can be tuned and controlled by external parameters like temperature, pumping, and injection electrons. Finally, in comparison with experimental measurements, we show that exciton emission in monolayer tungsten dichalcogenides is substantially reduced. This feature suggests that free exciton can be trapped in disordered potential wells to form a localized exciton and therefore offers a route toward novel optical properties.

  8. Excitons in single-walled carbon nanotubes: environmental effect

    International Nuclear Information System (INIS)

    Smyrnov, O.A.

    2010-01-01

    The properties of excitons in semiconducting single-walled carbon nanotubes (SWCNTs) isolated in vacuum or a medium and their contributions to the optical spectra of nanotubes are studied within the elementary potential model, in which an exciton is represented as a bound state of two oppositely charged quasiparticles confined to the nanotube surface. The emphasis is given on the influence of the dielectric environment surrounding a nanotube on the exciton spectra. For nanotubes in the environment with a permittivity less than ∼ 1:8; the ground-state exciton binding energies exceed the respective energy gaps, whereas the obtained binding energies of excitons in nanotubes in a medium with permittivity greater than ∼ 4 are in good accordance with the corresponding experimental data and consistent with the known scaling relation for the environmental effect. The stabilization of a single-electron spectrum in SWCNTs in media with rather low permittivities is discussed.

  9. Biexciton formation and exciton coherent coupling in layered GaSe

    Energy Technology Data Exchange (ETDEWEB)

    Dey, P.; Paul, J.; Stevens, C. E.; Glikin, N.; Karaiskaj, D., E-mail: karaiskaj@usf.edu [Department of Physics, University of South Florida, 4202 East Fowler Ave., Tampa, Florida 33620 (United States); Moody, G. [National Institute of Standards and Technology, 325 Broadway, Boulder, Colarado 80305 (United States); Kovalyuk, Z. D.; Kudrynskyi, Z. R. [Chernivtsi Department, Frantsevich Institute of Material Sciences Problems, The National Academy of Sciences of Ukraine, 5, Iryna Vilde St., 58001 Chernivtsi (Ukraine); Romero, A. H. [Physics Department, West Virginia University, Morgantown, West Virginia 26506-6315 (United States); Cantarero, A. [Materials Science Institute, University of Valencia, P.O. Box 2205, 46071 Valencia (Spain); Hilton, D. J. [Department of Physics, University of Alabama at Birmingham, Birmingham, Alabama 35294 (United States)

    2015-06-07

    Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ∼2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with “ab initio” theoretical calculations of the phonon spectra, indicate strong interaction with the A{sub 1}{sup ′} phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal.

  10. Biexciton formation and exciton coherent coupling in layered GaSe

    International Nuclear Information System (INIS)

    Dey, P.; Paul, J.; Stevens, C. E.; Glikin, N.; Karaiskaj, D.; Moody, G.; Kovalyuk, Z. D.; Kudrynskyi, Z. R.; Romero, A. H.; Cantarero, A.; Hilton, D. J.

    2015-01-01

    Nonlinear two-dimensional Fourier transform (2DFT) and linear absorption spectroscopy are used to study the electronic structure and optical properties of excitons in the layered semiconductor GaSe. At the 1s exciton resonance, two peaks are identified in the absorption spectra, which are assigned to splitting of the exciton ground state into the triplet and singlet states. 2DFT spectra acquired for co-linear polarization of the excitation pulses feature an additional peak originating from coherent energy transfer between the singlet and triplet. At cross-linear polarization of the excitation pulses, the 2DFT spectra expose a new peak likely originating from bound biexcitons. The polarization dependent 2DFT spectra are well reproduced by simulations using the optical Bloch equations for a four level system, where many-body effects are included phenomenologically. Although biexciton effects are thought to be strong in this material, only moderate contributions from bound biexciton creation can be observed. The biexciton binding energy of ∼2 meV was estimated from the separation of the peaks in the 2DFT spectra. Temperature dependent absorption and 2DFT measurements, combined with “ab initio” theoretical calculations of the phonon spectra, indicate strong interaction with the A 1 ′ phonon mode. Excitation density dependent 2DFT measurements reveal excitation induced dephasing and provide a lower limit for the homogeneous linewidth of the excitons in the present GaSe crystal

  11. Exciton management in organic photovoltaic multidonor energy cascades.

    Science.gov (United States)

    Griffith, Olga L; Forrest, Stephen R

    2014-05-14

    Multilayer donor regions in organic photovoltaics show improved power conversion efficiency when arranged in decreasing exciton energy order from the anode to the acceptor interface. These so-called "energy cascades" drive exciton transfer from the anode to the dissociating interface while reducing exciton quenching and allowing improved overlap with the solar spectrum. Here we investigate the relative importance of exciton transfer and blocking in a donor cascade employing diphenyltetracene (D1), rubrene (D2), and tetraphenyldibenzoperiflanthene (D3) whose optical gaps monotonically decrease from D1 to D3. In this structure, D1 blocks excitons from quenching at the anode, D2 accepts transfer of excitons from D1 and blocks excitons at the interface between D2 and D3, and D3 contributes the most to the photocurrent due to its strong absorption at visible wavelengths, while also determining the open circuit voltage. We observe singlet exciton Förster transfer from D1 to D2 to D3 consistent with cascade operation. The power conversion efficiency of the optimized cascade OPV with a C60 acceptor layer is 7.1 ± 0.4%, which is significantly higher than bilayer devices made with only the individual donors. We develop a quantitative model to identify the dominant exciton processes that govern the photocurrent generation in multilayer organic structures.

  12. Excitonic pathway to photoinduced magnetism in colloidal nanocrystals with nonmagnetic dopants.

    Science.gov (United States)

    Pinchetti, Valerio; Di, Qiumei; Lorenzon, Monica; Camellini, Andrea; Fasoli, Mauro; Zavelani-Rossi, Margherita; Meinardi, Francesco; Zhang, Jiatao; Crooker, Scott A; Brovelli, Sergio

    2018-02-01

    Electronic doping of colloidal semiconductor nanostructures holds promise for future device concepts in optoelectronic and spin-based technologies. Ag + is an emerging electronic dopant in III-V and II-VI nanostructures, introducing intragap electronic states optically coupled to the host conduction band. With its full 4d shell Ag + is nonmagnetic, and the dopant-related luminescence is ascribed to decay of the conduction-band electron following transfer of the photoexcited hole to Ag + . This optical activation process and the associated modification of the electronic configuration of Ag + remain unclear. Here, we trace a comprehensive picture of the excitonic process in Ag-doped CdSe nanocrystals and demonstrate that, in contrast to expectations, capture of the photohole leads to conversion of Ag + to paramagnetic Ag 2+ . The process of exciton recombination is thus inextricably tied to photoinduced magnetism. Accordingly, we observe strong optically activated magnetism and diluted magnetic semiconductor behaviour, demonstrating that optically switchable magnetic nanomaterials can be obtained by exploiting excitonic processes involving nonmagnetic impurities.

  13. Accessing the dark exciton spin in deterministic quantum-dot microlenses

    Science.gov (United States)

    Heindel, Tobias; Thoma, Alexander; Schwartz, Ido; Schmidgall, Emma R.; Gantz, Liron; Cogan, Dan; Strauß, Max; Schnauber, Peter; Gschrey, Manuel; Schulze, Jan-Hindrik; Strittmatter, Andre; Rodt, Sven; Gershoni, David; Reitzenstein, Stephan

    2017-12-01

    The dark exciton state in semiconductor quantum dots (QDs) constitutes a long-lived solid-state qubit which has the potential to play an important role in implementations of solid-state-based quantum information architectures. In this work, we exploit deterministically fabricated QD microlenses which promise enhanced photon extraction, to optically prepare and read out the dark exciton spin and observe its coherent precession. The optical access to the dark exciton is provided via spin-blockaded metastable biexciton states acting as heralding states, which are identified by deploying polarization-sensitive spectroscopy as well as time-resolved photon cross-correlation experiments. Our experiments reveal a spin-precession period of the dark exciton of (0.82 ± 0.01) ns corresponding to a fine-structure splitting of (5.0 ± 0.7) μeV between its eigenstates |↑ ⇑ ±↓ ⇓ ⟩. By exploiting microlenses deterministically fabricated above pre-selected QDs, our work demonstrates the possibility to scale up implementations of quantum information processing schemes using the QD-confined dark exciton spin qubit, such as the generation of photonic cluster states or the realization of a solid-state-based quantum memory.

  14. Energy and Information Transfer Via Coherent Exciton Wave Packets

    Science.gov (United States)

    Zang, Xiaoning

    associated excitations were dubbed twisted excitons. Twisted exciton packets can be manipulated as they travel down molecular chains, and this has applications in quantum information science as well. In each setting considered, exciton dynamics were initially studied using a simple tight-binding formalism. This misses the actual many-body interactions and multiple energy levels associated real systems. To remedy this, I adapted an existing time-domain Density Functional Theory code and applied it to study the dynamics of exciton wave packets on quasi-one-dimensional systems. This required the use of high-performance computing and the construction of a number of key auxiliary codes. Establishing the requisite methodology constituted a substantial part of the entire thesis. Surprisingly, this effort uncovered a computational issue associated with Rabi oscillations that had been incorrectly characterized in the literature. My research elucidated the actual problem and a solution was found. This new methodology was an integral part of the overall computational analysis. The thesis then takes up the a detailed consideration of the prospect for creating systems that support a strong measure of transport coherence. While physical implementations include molecular assemblies, solid-state superlattices, and even optical lattices, I decided to focus on assemblies of nanometer-sized silicon quantum dots. First principles computational analysis was used to quantify reorganization within individual dots and excitonic coupling between dots. Quantum dot functionalizations were identified that make it plausible to maintain a measure of excitonic coherence even at room temperatures. Attention was then turned to the use of covalently bonded bridge material to join quantum dots in a way that facilitates efficient exciton transfer. Both carbon and silicon structures were considered by considering the way in which subunits might be best brought together. This resulted in a set of design criteria

  15. Picosecond dynamics of internal exciton transitions in CdSe nanorods

    DEFF Research Database (Denmark)

    Cooke, D. G.; Jepsen, Peter Uhd; Lek, Jun Yan

    2013-01-01

    . The onset of exciton-LO phonon coupling appears as a bleach in the optical conductivity spectra at the LO phonon energy for times > 1 ps after excitation. Simulations show a suppressed exciton temperature due to thermally excited hole states being rapidly captured onto ligands or unpassivated surface states...

  16. Reconstructing Space- and Energy-Dependent Exciton Generation in Solution-Processed Inverted Organic Solar Cells.

    Science.gov (United States)

    Wang, Yuheng; Zhang, Yajie; Lu, Guanghao; Feng, Xiaoshan; Xiao, Tong; Xie, Jing; Liu, Xiaoyan; Ji, Jiahui; Wei, Zhixiang; Bu, Laju

    2018-04-25

    Photon absorption-induced exciton generation plays an important role in determining the photovoltaic properties of donor/acceptor organic solar cells with an inverted architecture. However, the reconstruction of light harvesting and thus exciton generation at different locations within organic inverted device are still not well resolved. Here, we investigate the film depth-dependent light absorption spectra in a small molecule donor/acceptor film. Including depth-dependent spectra into an optical transfer matrix method allows us to reconstruct both film depth- and energy-dependent exciton generation profiles, using which short-circuit current and external quantum efficiency of the inverted device are simulated and compared with the experimental measurements. The film depth-dependent spectroscopy, from which we are able to simultaneously reconstruct light harvesting profile, depth-dependent composition distribution, and vertical energy level variations, provides insights into photovoltaic process. In combination with appropriate material processing methods and device architecture, the method proposed in this work will help optimizing film depth-dependent optical/electronic properties for high-performance solar cells.

  17. Exciton Mapping at Subwavelength Scales in Two-Dimensional Materials

    KAUST Repository

    Tizei, Luiz H. G.

    2015-03-01

    Spatially resolved electron-energy-loss spectroscopy (EELS) is performed at diffuse interfaces between MoS2 and MoSe2 single layers. With a monochromated electron source (20 meV) we successfully probe excitons near the interface by obtaining the low loss spectra at the nanometer scale. The exciton maps clearly show variations even with a 10 nm separation between measurements; consequently, the optical band gap can be measured with nanometer-scale resolution, which is 50 times smaller than the wavelength of the emitted photons. By performing core-loss EELS at the same regions, we observe that variations in the excitonic signature follow the chemical composition. The exciton peaks are observed to be broader at interfaces and heterogeneous regions, possibly due to interface roughness and alloying effects. Moreover, we do not observe shifts of the exciton peak across the interface, possibly because the interface width is not much larger than the exciton Bohr radius.

  18. The nonlinear optical properties of a magneto-exciton in a strained Ga0.2In0.8As/GaAs quantum dot

    International Nuclear Information System (INIS)

    Kumar, N. R. Senthil; Peter, A. John; Yoo Chang Kyoo

    2013-01-01

    The magnetic field-dependent heavy hole excitonic states in a strained Ga 0.2 In 0.8 As/GaAs quantum dot are investigated by taking into account the anisotropy, non-parabolicity of the conduction band, and the geometrical confinement. The strained quantum dot is considered as a parabolic dot of InAs embedded in a GaAs barrier material. The dependence of the effective excitonic g-factor as a function of dot radius and the magnetic field strength is numerically measured. The interband optical transition energy as a function of geometrical confinement is computed in the presence of a magnetic field. The magnetic field-dependent oscillator strength of interband transition under the geometrical confinement is studied. The exchange enhancements as a function of dot radius are observed for various magnetic field strengths in a strained Ga 0.2 In 0.8 As/GaAs quantum dot. Heavy hole excitonic absorption spectra, the changes in refractive index, and the third-order susceptibility of third-order harmonic generation are investigated in the Ga 0.2 In 0.8 As/GaAs quantum dot. The result shows that the effect of magnetic field strength is more strongly dependent on the nonlinear optical property in a low-dimensional semiconductor system. (condensed matter: electronic structure, electrical, magnetic, and optical properties)

  19. Optical pumping and negative luminescence polarization in charged GaAs quantum dots

    Science.gov (United States)

    Shabaev, Andrew; Stinaff, Eric A.; Bracker, Allan S.; Gammon, Daniel; Efros, Alexander L.; Korenev, Vladimir L.; Merkulov, Igor

    2009-01-01

    Optical pumping of electron spins and negative photoluminescence polarization are observed when interface quantum dots in a GaAs quantum well are excited nonresonantly by circularly polarized light. Both observations can be explained by the formation of long-lived dark excitons through hole spin relaxation in the GaAs quantum well prior to exciton capture. In this model, optical pumping of resident electron spins is caused by capture of dark excitons and recombination in charged quantum dots. Negative polarization results from accumulation of dark excitons in the quantum well and is enhanced by optical pumping. The dark exciton model describes the experimental results very well, including intensity and bias dependence of the photoluminescence polarization and the Hanle effect.

  20. Excitonic terahertz photoconductivity in intrinsic semiconductor nanowires

    Science.gov (United States)

    Yan, Jie-Yun

    2018-06-01

    Excitonic terahertz photoconductivity in intrinsic semiconductor nanowires is studied. Based on the excitonic theory, the numerical method to calculate the photoconductivity spectrum in the nanowires is developed, which can simulate optical pump terahertz-probe spectroscopy measurements on real nanowires and thereby calculate the typical photoconductivity spectrum. With the help of the energetic structure deduced from the calculated linear absorption spectrum, the numerically observed shift of the resonant peak in the photoconductivity spectrum is found to result from the dominant exciton transition between excited or continuum states to the ground state, and the quantitative analysis is in good agreement with the quantum plasmon model. Besides, the dependence of the photoconductivity on the polarization of the terahertz field is also discussed. The numerical method and supporting theoretical analysis provide a new tool for experimentalists to understand the terahertz photoconductivity in intrinsic semiconductor nanowires at low temperatures or for nanowires subjected to below bandgap photoexcitation, where excitonic effects dominate.

  1. Resonant Rayleigh scattering of exciton-polaritons in multiple quantum wells

    DEFF Research Database (Denmark)

    Malpuech, Guillaume; Kavokin, Alexey; Langbein, Wolfgang Werner

    2000-01-01

    A theoretical concept of resonant Rayleigh scattering (RRS) of exciton-polaritons in multiple quantum wells (QWs) is presented. The optical coupling between excitons in different QWs can strongly affect the RRS dynamics, giving rise to characteristic temporal oscillations on a picosecond scale....... Bragg and anti-Bragg arranged QW structures with the same excitonic parameters are predicted to have drastically different RRS spectra. Experimental data on the RRS from multiple QWs show the predicted strong temporal oscillations at small scattering angles, which are well explained by the presented...

  2. Interlayer excitons in a bulk van der Waals semiconductor.

    Science.gov (United States)

    Arora, Ashish; Drüppel, Matthias; Schmidt, Robert; Deilmann, Thorsten; Schneider, Robert; Molas, Maciej R; Marauhn, Philipp; Michaelis de Vasconcellos, Steffen; Potemski, Marek; Rohlfing, Michael; Bratschitsch, Rudolf

    2017-09-21

    Bound electron-hole pairs called excitons govern the electronic and optical response of many organic and inorganic semiconductors. Excitons with spatially displaced wave functions of electrons and holes (interlayer excitons) are important for Bose-Einstein condensation, superfluidity, dissipationless current flow, and the light-induced exciton spin Hall effect. Here we report on the discovery of interlayer excitons in a bulk van der Waals semiconductor. They form due to strong localization and spin-valley coupling of charge carriers. By combining high-field magneto-reflectance experiments and ab initio calculations for 2H-MoTe 2 , we explain their salient features: the positive sign of the g-factor and the large diamagnetic shift. Our investigations solve the long-standing puzzle of positive g-factors in transition metal dichalcogenides, and pave the way for studying collective phenomena in these materials at elevated temperatures.Excitons, quasi-particles of bound electron-hole pairs, are at the core of the optoelectronic properties of layered transition metal dichalcogenides. Here, the authors unveil the presence of interlayer excitons in bulk van der Waals semiconductors, arising from strong localization and spin-valley coupling of charge carriers.

  3. Excitonic spectrum of the ZnO/ZnMgO quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Bobrov, M. A., E-mail: largaseal@gmail.com; Toropov, A. A.; Ivanov, S. V. [Russian Academy of Sciences, Ioffe Physical Technical Institute (Russian Federation); El-Shaer, A.; Bakin, A.; Waag, A. [TU Braunschweig, Institute of Semiconductor Technology (Germany)

    2011-06-15

    Excitonic spectrum of the wurtzite ZnO/Zn{sub 1-x}Mg{sub x}O quantum wells with a width on the order of or larger than the Bohr radius of the exciton has been studied; the quantum wells have been grown by the method of molecular beam epitaxy (with plasma-assisted activation of oxygen) on substrates of sapphire (0001). Low-temperature (25 K) spectra of photoluminescence excitation (PLE) have been experimentally measured, making it possible to resolve the peaks of exciton absorption in the quantum well. The spectrum of excitons in the quantum well is theoretically determined as a result of numerical solution of the Schroedinger equation by the variational method. The value of elastic stresses in the structure (used in calculations) has been determined from theoretical simulation of measured spectra of optical reflection. A comparison of experimental data with the results of calculations makes it possible to relate the observed features in the PLE spectra to excitons, including the lower level of dimensional quantization for electrons and two first levels of holes for the A and B valence bands of the wurtzite crystal. The values of the electron and hole masses in ZnO are refined, and the value of the built-in electric field introduced by spontaneous and piezoelectric polarizations is estimated.

  4. Anomalous behavior of the excited state of the A exciton in bulk WS2

    DEFF Research Database (Denmark)

    Jindal, Vishwas; Bhuyan, Sumi; Deilmann, Thorsten

    2018-01-01

    Results of optical spectroscopy studies on bulk 2H-WS2 at energies close to its direct band gap are presented. Reflectance and absorption measurements at low temperature show only one dominant feature due to the A exciton of bulk WS2 at similar to 2.02 eV. However, a laser-modulated photoreflecta......Results of optical spectroscopy studies on bulk 2H-WS2 at energies close to its direct band gap are presented. Reflectance and absorption measurements at low temperature show only one dominant feature due to the A exciton of bulk WS2 at similar to 2.02 eV. However, a laser....... The experimental results are analyzed by comparison with many-body perturbation theory calculations, including the solutions of the Bethe-Salpeter equation. A* is identified as the first excited state of the A exciton, that is, A(n = 2). The anomalous behavior of A* is explained by its distinct wave function...... spread along the c axis, the direction of weak van der Waals bonding, which makes it more susceptible to perturbations. Our ab initio calculations suggest that the A exciton in the ground state has a two-dimensional (2D) nature with a large binding energy E-b, in fair agreement with E-b similar to 90...

  5. Field-modulation spectroscopy of pentacene thin films using field-effect devices: Reconsideration of the excitonic structure

    Science.gov (United States)

    Haas, Simon; Matsui, Hiroyuki; Hasegawa, Tatsuo

    2010-10-01

    We report pure electric-field effects on the excitonic absorbance of pentacene thin films as measured by unipolar field-effect devices that allowed us to separate the charge accumulation effects. The field-modulated spectra between 1.8 and 2.6 eV can be well fitted with the first derivative curve of Frenkel exciton absorption and its vibronic progression, and at higher energy a field-induced feature appears at around 2.95 eV. The results are in sharp contrast to the electroabsorption spectra reported by Sebastian in previous studies [Chem. Phys. 61, 125 (1981)10.1016/0301-0104(81)85055-0], and leads us to reconsider the excitonic structure including the location of charge-transfer excitons. Nonlinear π -electronic response is discussed based on second-order electro-optic (Kerr) spectra.

  6. Exciton diffusion in WSe2 monolayers embedded in a van der Waals heterostructure

    Science.gov (United States)

    Cadiz, F.; Robert, C.; Courtade, E.; Manca, M.; Martinelli, L.; Taniguchi, T.; Watanabe, K.; Amand, T.; Rowe, A. C. H.; Paget, D.; Urbaszek, B.; Marie, X.

    2018-04-01

    We have combined spatially resolved steady-state micro-photoluminescence with time-resolved photoluminescence to investigate the exciton diffusion in a WSe2 monolayer encapsulated with hexagonal boron nitride. At 300 K, we extract an exciton diffusion length of LX = 0.36 ± 0.02 μm and an exciton diffusion coefficient of DX = 14.5 ± 2 cm2/s. This represents a nearly 10-fold increase in the effective mobility of excitons with respect to several previously reported values on nonencapsulated samples. At cryogenic temperatures, the high optical quality of these samples has allowed us to discriminate the diffusion of the different exciton species: bright and dark neutral excitons, as well as charged excitons. The longer lifetime of dark neutral excitons yields a larger diffusion length of LXD=1.5 ±0.02 μ m.

  7. Angular momentum transport with twisted exciton wave packets

    Science.gov (United States)

    Zang, Xiaoning; Lusk, Mark T.

    2017-10-01

    A chain of cofacial molecules with CN or CN h symmetry supports excitonic states with a screwlike structure. These can be quantified with the combination of an axial wave number and an azimuthal winding number. Combinations of these states can be used to construct excitonic wave packets that spiral down the chain with well-determined linear and angular momenta. These twisted exciton wave packets can be created and annihilated using laser pulses, and their angular momentum can be optically modified during transit. This allows for the creation of optoexcitonic circuits in which information, encoded in the angular momentum of light, is converted into excitonic wave packets that can be manipulated, transported, and then reemitted. A tight-binding paradigm is used to demonstrate the key ideas. The approach is then extended to quantify the evolution of twisted exciton wave packets in a many-body, multilevel time-domain density functional theory setting. In both settings, numerical methods are developed that allow the site-to-site transfer of angular momentum to be quantified.

  8. Exciton broadening in WS2 /graphene heterostructures

    International Nuclear Information System (INIS)

    Hill, Heather M.; Rigosi, Albert F.; Raja, Archana

    2017-01-01

    Here, we have used optical spectroscopy to observe spectral broadening of WS 2 exciton reflectance peaks in heterostructures of monolayer WS 2 capped with mono- to few-layer graphene. The broadening is found to be similar for the A and B excitons and on the order of 5–10 meV. No strong dependence on the number of graphene layers was observed within experimental uncertainty. The broadening can be attributed to charge- and energy-transfer processes between the two materials, providing an observed lower bound for the corresponding time scales of 65 fs.

  9. Well separated trion and neutral excitons on superacid treated MoS{sub 2} monolayers

    Energy Technology Data Exchange (ETDEWEB)

    Cadiz, Fabian, E-mail: cadiz@insa-toulouse.fr; Tricard, Simon; Gay, Maxime; Lagarde, Delphine; Wang, Gang; Robert, Cedric; Renucci, Pierre; Urbaszek, Bernhard; Marie, Xavier [Université de Toulouse, INSA-CNRS-UPS, LPCNO, 135 Av. Rangueil, 31077 Toulouse (France)

    2016-06-20

    Developments in optoelectronics and spin-optronics based on transition metal dichalcogenide monolayers (MLs) need materials with efficient optical emission and well-defined transition energies. In as-exfoliated MoS{sub 2} MLs, the photoluminescence (PL) spectra even at low temperature consist typically of broad, overlapping contributions from neutral, charged excitons (trions) and localized states. Here, we show that in superacid treated MoS{sub 2} MLs, the PL intensity increases by up to 60 times at room temperature. The neutral and charged exciton transitions are spectrally well separated in PL and reflectivity at T = 4 K, with linewidth for the neutral exciton of 15 meV, but both transitions have similar intensities compared to the ones in as-exfoliated MLs at the same temperature. Time resolved experiments uncover picoseconds recombination dynamics analyzed separately for charged and neutral exciton emissions. Using the chiral interband selection rules, we demonstrate optically induced valley polarization for both complexes and valley coherence for only the neutral exciton.

  10. Ultrafast dynamics of confined and localised excitons and biexcitons in low-dimensional semiconductors

    DEFF Research Database (Denmark)

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

    1999-01-01

    Coherent optical spectroscopy in the form of nonlinear transient four-wave mixing (TFWM) and linear resonant Rayleigh scattering (RRS) has been applied to investigate the exciton dynamics of low-dimensional semiconductor heterostructures. The dephasing times of excitons are determined from...

  11. Optical conductivity calculation of a k.p model semiconductor GaAs incorporating first-order electron-hole vertex correction

    Science.gov (United States)

    Nurhuda, Maryam; Aziz Majidi, Muhammad

    2018-04-01

    The role of excitons in semiconducting materials carries potential applications. Experimental results show that excitonic signals also appear in optical absorption spectra of semiconductor system with narrow gap, such as Gallium Arsenide (GaAs). While on the theoretical side, calculation of optical spectra based purely on Density Functional Theory (DFT) without taking electron-hole (e-h) interactions into account does not lead to the appearance of any excitonic signal. Meanwhile, existing DFT-based algorithms that include a full vertex correction through Bethe-Salpeter equation may reveal an excitonic signal, but the algorithm has not provided a way to analyze the excitonic signal further. Motivated to provide a way to isolate the excitonic effect in the optical response theoretically, we develop a method of calculation for the optical conductivity of a narrow band-gap semiconductor GaAs within the 8-band k.p model that includes electron-hole interactions through first-order electron-hole vertex correction. Our calculation confirms that the first-order e-h vertex correction reveals excitonic signal around 1.5 eV (the band gap edge), consistent with the experimental data.

  12. Visualising Berry phase and diabolical points in a quantum exciton-polariton billiard.

    Science.gov (United States)

    Estrecho, E; Gao, T; Brodbeck, S; Kamp, M; Schneider, C; Höfling, S; Truscott, A G; Ostrovskaya, E A

    2016-11-25

    Diabolical points (spectral degeneracies) can naturally occur in spectra of two-dimensional quantum systems and classical wave resonators due to simple symmetries. Geometric Berry phase is associated with these spectral degeneracies. Here, we demonstrate a diabolical point and the corresponding Berry phase in the spectrum of hybrid light-matter quasiparticles-exciton-polaritons in semiconductor microcavities. It is well known that sufficiently strong optical pumping can drive exciton-polaritons to quantum degeneracy, whereby they form a macroscopically populated quantum coherent state similar to a Bose-Einstein condensate. By pumping a microcavity with a spatially structured light beam, we create a two-dimensional quantum billiard for the exciton-polariton condensate and demonstrate a diabolical point in the spectrum of the billiard eigenstates. The fully reconfigurable geometry of the potential walls controlled by the optical pump enables a striking experimental visualization of the Berry phase associated with the diabolical point. The Berry phase is observed and measured by direct imaging of the macroscopic exciton-polariton probability densities.

  13. Exciton Scattering approach for conjugated macromolecules: from electronic spectra to electron-phonon coupling

    Science.gov (United States)

    Tretiak, Sergei

    2014-03-01

    The exciton scattering (ES) technique is a multiscale approach developed for efficient calculations of excited-state electronic structure and optical spectra in low-dimensional conjugated macromolecules. Within the ES method, the electronic excitations in the molecular structure are attributed to standing waves representing quantum quasi-particles (excitons), which reside on the graph. The exciton propagation on the linear segments is characterized by the exciton dispersion, whereas the exciton scattering on the branching centers is determined by the energy-dependent scattering matrices. Using these ES energetic parameters, the excitation energies are then found by solving a set of generalized ``particle in a box'' problems on the graph that represents the molecule. All parameters can be extracted from quantum-chemical computations of small molecular fragments and tabulated in the ES library for further applications. Subsequently, spectroscopic modeling for any macrostructure within considered molecular family could be performed with negligible numerical effort. The exciton scattering properties of molecular vertices can be further described by tight-binding or equivalently lattice models. The on-site energies and hopping constants are obtained from the exciton dispersion and scattering matrices. Such tight-binding model approach is particularly useful to describe the exciton-phonon coupling, energetic disorder and incoherent energy transfer in large branched conjugated molecules. Overall the ES applications accurately reproduce the optical spectra compared to the reference quantum chemistry results, and make possible to predict spectra of complex macromolecules, where conventional electronic structure calculations are unfeasible.

  14. Exciton-plasmon coupling interactions: from principle to applications

    Science.gov (United States)

    Cao, En; Lin, Weihua; Sun, Mengtao; Liang, Wenjie; Song, Yuzhi

    2018-01-01

    The interaction of exciton-plasmon coupling and the conversion of exciton-plasmon-photon have been widely investigated experimentally and theoretically. In this review, we introduce the exciton-plasmon interaction from basic principle to applications. There are two kinds of exciton-plasmon coupling, which demonstrate different optical properties. The strong exciton-plasmon coupling results in two new mixed states of light and matter separated energetically by a Rabi splitting that exhibits a characteristic anticrossing behavior of the exciton-LSP energy tuning. Compared to strong coupling, such as surface-enhanced Raman scattering, surface plasmon (SP)-enhanced absorption, enhanced fluorescence, or fluorescence quenching, there is no perturbation between wave functions; the interaction here is called the weak coupling. SP resonance (SPR) arises from the collective oscillation induced by the electromagnetic field of light and can be used for investigating the interaction between light and matter beyond the diffraction limit. The study on the interaction between SPR and exaction has drawn wide attention since its discovery not only due to its contribution in deepening and broadening the understanding of SPR but also its contribution to its application in light-emitting diodes, solar cells, low threshold laser, biomedical detection, quantum information processing, and so on.

  15. Excitons in Single-Walled Carbon Nanotubes and Their Dynamics

    Science.gov (United States)

    Amori, Amanda R.; Hou, Zhentao; Krauss, Todd D.

    2018-04-01

    Understanding exciton dynamics in single-walled carbon nanotubes (SWCNTs) is essential to unlocking the many potential applications of these materials. This review summarizes recent progress in understanding exciton photophysics and, in particular, exciton dynamics in SWCNTs. We outline the basic physical and electronic properties of SWCNTs, as well as bright and dark transitions within the framework of a strongly bound one-dimensional excitonic model. We discuss the many facets of ultrafast carrier dynamics in SWCNTs, including both single-exciton states (bright and dark) and multiple-exciton states. Photophysical properties that directly relate to excitons and their dynamics, including exciton diffusion lengths, chemical and structural defects, environmental effects, and photoluminescence photon statistics as observed through photon antibunching measurements, are also discussed. Finally, we identify a few key areas for advancing further research in the field of SWCNT excitons and photonics.

  16. Effects of surface and interface traps on exciton and multi-exciton dynamics in core/shell quantum dots

    Science.gov (United States)

    Bozio, Renato; Righetto, Marcello; Minotto, Alessandro

    2017-08-01

    Exciton interactions and dynamics are the most important factors determining the exceptional photophysical properties of semiconductor quantum dots (QDs). In particular, best performances have been obtained for ingeniously engineered core/shell QDs. We have studied two factors entering in the exciton decay dynamics with adverse effects for the luminescence efficiency: exciton trapping at surface and interface traps, and non-radiative Auger recombination in QDs carrying either net charges or multiple excitons. In this work, we present a detailed study into the optical absorption, fluorescence dynamics and quantum yield, as well as ultrafast transient absorption properties of CdSe/CdS, CdSe/Cd0.5Zn0.5S, and CdSe/ZnS QDs as a function of shell thickness. It turns out that de-trapping processes play a pivotal role in determining steady state emission properties. By studying the excitation dependent photoluminescence quantum yields (PLQY) in different CdSe/CdxZn1-xS (x = 0, 0.5, 1) QDs, we demonstrate the different role played by hot and cold carrier trapping rates in determining fluorescence quantum yields. Finally, the use of global analysis allows us untangling the complex ultrafast transient absorption signals. Smoothing of interface potential, together with effective surface passivation, appear to be crucial factors in slowing down both Auger-based and exciton trapping recombination processes.

  17. Anisotropic Exciton Rabi Oscillation in Single Telecommunication-Band Quantum Dot

    Science.gov (United States)

    Toshiyuki Miyazawa,; Toshihiro Nakaoka,; Katsuyuki Watanabe,; Naoto Kumagai,; Naoki Yokoyama,; Yasuhiko Arakawa,

    2010-06-01

    Anisotropic Rabi oscillation in the exciton state in a single InAs/GaAs quantum dot (QD) was demonstrated in the telecommunication-band by selecting two orthogonal polarization angles of the excitation laser. Our InAs QDs were embedded in an intrinsic layer of an n-i-Schottky diode, which provides an electric field to extract photoexcited carriers from QDs. Owing to the potential anisotropy of QDs, the fine structure splitting (FSS) energy in the exciton state in single InAs QDs was ˜110 μeV, measured by polarization-resolved photocurrent spectroscopy. The ratio between two different Rabi frequencies, which reflect anisotropic dipole moments of two orthogonal exciton states, was estimated to be ˜1.2. This demonstrates that the selective control of two orthogonal polarized exciton states is a promising technique for exciton-based-quantum information devices compatible with fiber optics.

  18. Scaling laws of Rydberg excitons

    Science.gov (United States)

    Heckötter, J.; Freitag, M.; Fröhlich, D.; Aßmann, M.; Bayer, M.; Semina, M. A.; Glazov, M. M.

    2017-09-01

    Rydberg atoms have attracted considerable interest due to their huge interaction among each other and with external fields. They demonstrate characteristic scaling laws in dependence on the principal quantum number n for features such as the magnetic field for level crossing or the electric field of dissociation. Recently, the observation of excitons in highly excited states has allowed studying Rydberg physics in cuprous oxide crystals. Fundamentally different insights may be expected for Rydberg excitons, as the crystal environment and associated symmetry reduction compared to vacuum give not only optical access to many more states within an exciton multiplet but also extend the Hamiltonian for describing the exciton beyond the hydrogen model. Here we study experimentally and theoretically the scaling of several parameters of Rydberg excitons with n , for some of which we indeed find laws different from those of atoms. For others we find identical scaling laws with n , even though their origin may be distinctly different from the atomic case. At zero field the energy splitting of a particular multiplet n scales as n-3 due to crystal-specific terms in the Hamiltonian, e.g., from the valence band structure. From absorption spectra in magnetic field we find for the first crossing of levels with adjacent principal quantum numbers a Br∝n-4 dependence of the resonance field strength, Br, due to the dominant paramagnetic term unlike for atoms for which the diamagnetic contribution is decisive, resulting in a Br∝n-6 dependence. By contrast, the resonance electric field strength shows a scaling as Er∝n-5 as for Rydberg atoms. Also similar to atoms with the exception of hydrogen we observe anticrossings between states belonging to multiplets with different principal quantum numbers at these resonances. The energy splittings at the avoided crossings scale roughly as n-4, again due to crystal specific features in the exciton Hamiltonian. The data also allow us to

  19. Excitonic and photonic processes in materials

    CERN Document Server

    Williams, Richard

    2015-01-01

    This book is expected to present state-of-the-art understanding of a selection of excitonic and photonic processes in useful materials from semiconductors to insulators to metal/insulator nanocomposites, both inorganic and organic.  Among the featured applications are components of solar cells, detectors, light-emitting devices, scintillators, and materials with novel optical properties.  Excitonic properties are particularly important in organic photovoltaics and light emitting devices, as also in questions of the ultimate resolution and efficiency of new-generation scintillators for medical diagnostics,  border security, and nuclear nonproliferation.  Novel photonic and optoelectronic applications benefit from new material combinations and structures to be discussed.

  20. Large-k exciton dynamics in GaN epilayers: Nonthermal and thermal regimes

    Science.gov (United States)

    Vinattieri, Anna; Bogani, Franco; Cavigli, Lucia; Manzi, Donatella; Gurioli, Massimo; Feltin, Eric; Carlin, Jean-François; Martin, Denis; Butté, Raphaël; Grandjean, Nicolas

    2013-02-01

    We present a detailed investigation performed at low temperature (T<50 K) concerning the exciton dynamics in GaN epilayers grown on c-plane sapphire substrates, focusing on the exciton formation and the transition from the nonthermal to the thermal regime. The time-resolved kinetics of longitudinal-optical-phonon replicas is used to address the energy relaxation in the excitonic band. From picosecond time-resolved spectra, we bring evidence for a long lasting nonthermal excitonic distribution, which accounts for the first 50 ps. Such a behavior is confirmed in different experimental conditions when both nonresonant and resonant excitations are used. At low excitation power density, the exciton formation and their subsequent thermalization are dominated by impurity scattering rather than by acoustic phonon scattering. The estimate of the average energy of the excitons as a function of delay after the excitation pulse provides information on the relaxation time, which describes the evolution of the exciton population to the thermal regime.

  1. Resolving ultrafast exciton migration in organic solids at the nanoscale

    Science.gov (United States)

    Ginsberg, Naomi

    The migration of Frenkel excitons, tightly-bound electron-hole pairs, in photosynthesis and in organic semiconducting films is critical to the efficiency of natural and artificial light harvesting. While these materials exhibit a high degree of structural heterogeneity on the nanoscale, traditional measurements of exciton migration lengths are performed on bulk samples. Since both the characteristic length scales of structural heterogeneity and the reported bulk diffusion lengths are smaller than the optical diffraction limit, we adapt far-field super-resolution fluorescence imaging to uncover the correlations between the structural and energetic landscapes that the excitons explore. By combining the ultrafast super-resolved measurements with exciton hopping simulations we furthermore specify the nature (in addition to the extent) of exciton migration as a function of the intrinsic and ensemble chromophore energy scales that determine a spatio-energetic landscape for migration. In collaboration with: Samuel Penwell, Lucas Ginsberg, University of California, Berkeley and Rodrigo Noriega University of Utah.

  2. How to Draw Energy Level Diagrams in Excitonic Solar Cells.

    Science.gov (United States)

    Zhu, X-Y

    2014-07-03

    Emerging photovoltaic devices based on molecular and nanomaterials are mostly excitonic in nature. The initial absorption of a photon in these materials creates an exciton that can subsequently dissociate in each material or at their interfaces to give charge carriers. Any attempt at mechanistic understanding of excitonic solar cells must start with drawing energy level diagrams. This seemingly elementary exercise, which is described in textbooks for inorganic solar cells, has turned out to be a difficult subject in the literature. The problem stems from conceptual confusion of single-particle energy with quasi-particle energy and the misleading practice of mixing the two on the same energy level diagram. Here, I discuss how to draw physically accurate energy diagrams in excitonic solar cells using only single-particle energies (ionization potentials and electron affinities) of both ground and optically excited states. I will briefly discuss current understanding on the electronic energy landscape responsible for efficient charge separation in excitonic solar cells.

  3. Excitonic effects and related properties in semiconductor nanostructures: roles of size and dimensionality

    Science.gov (United States)

    Wu, Shudong; Cheng, Liwen; Wang, Qiang

    2017-08-01

    The size- and dimensionality-dependence of excitonic effects and related properties in semiconductor nanostructures are theoretically studied in detail within the effective-mass approximation. When nanostructure sizes become smaller than the bulk exciton Bohr radius, excitonic effects are significantly enhanced with reducing size or dimensionality. This is as a result of quantum confinement in more directions leading to larger exciton binding energies and normalized exciton oscillator strengths. These excitonic effects originate from electron-hole Coulombic interactions, which strongly enhance the oscillator strength between the electron and hole. It is also established that the universal scaling of exciton binding energy versus the inverse of the exciton Bohr radius follows a linear scaling law. Herein, we propose a stretched exponential law for the size scaling of optical gap, which is in good agreement with the calculated data. Due to differences in the confinement dimensionality, the radiative lifetime of low-dimensional excitons becomes shorter than that of bulk excitons. The size dependence of the exciton radiative lifetimes is in good agreement with available experimental data. This strongly enhanced electron-hole exchange interaction is expected in low-dimensional structures due to enriched excitonic effects. The main difference in nanostructures compared to the bulk can be interpreted in terms of the enhanced excitonic effects induced by exciton localization. The enhanced excitonic effects are expected to be of importance in developing stable and high-efficiency nanoscale excitonic optoelectronic devices.

  4. Geometrical-confinement effects on excitons in quantum disks

    International Nuclear Information System (INIS)

    Song, J.; Ulloa, S.E.

    1995-01-01

    Excitons confined to flat semiconductor quantum dots with elliptical cross sections are considered as we study geometrical effects on exciton binding energy, electron-hole separation, and the resulting linear optical properties. We use numerical matrix diagonalization techniques with appropriately large and optimized basis sets in an effective-mass Hamiltonian approach. The linear optical susceptibilities of GaAs and InAs dots for several different size ratios are discussed and compared to experimental photoluminescence spectra obtained on GaAs/Al x Ga 1-x As and InAs/GaAs quantum dots. For quantum dots of several nm in size, there is a strong blueshift of the luminescence due to geometrical-confinement effects. Also, transition peaks are split and shifted towards higher energy, in comparison with dots with circular cross sections

  5. Vibronic effects and destruction of exciton coherence in optical spectra of J-aggregates: A variational polaron transformation approach

    Energy Technology Data Exchange (ETDEWEB)

    Bloemsma, E.A.; Silvis, M.H.; Stradomska, A.; Knoester, J., E-mail: j.knoester@rug.nl

    2016-12-20

    Using a symmetry adapted polaron transformation of the Holstein Hamiltonian, we study the interplay of electronic excitation-vibration couplings, resonance excitation transfer interactions, and temperature in the linear absorption spectra of molecular J-aggregates. Semi-analytical expressions for the spectra are derived and compared with results obtained from direct numerical diagonalization of the Hamiltonian in the two-particle basis set representation. At zero temperature, we show that our polaron transformation reproduces both the collective (exciton) and single-molecule (vibrational) optical response associated with the appropriate standard perturbation limits. Specifically, for the molecular dimer excellent agreement with the spectra from the two-particle approach for the entire range of model parameters is obtained. This is in marked contrast to commonly used polaron transformations. Upon increasing the temperature, the spectra show a transition from the collective to the individual molecular features, which results from the thermal destruction of the exciton coherence.

  6. Effect of interface disorder on quantum well excitons and microcavity polaritons

    International Nuclear Information System (INIS)

    Savona, Vincenzo

    2007-01-01

    The theory of the linear optical response of excitons in quantum wells and polaritons in planar semiconductor microcavities is reviewed, in the light of the existing experiments. For quantum well excitons, it is shown that disorder mainly affects the exciton centre-of-mass motion and is modelled by an effective Schroedinger equation in two dimensions. For polaritons, a unified model accounting for quantum well roughness and fluctuations of the microcavity thickness is developed. Numerical results confirm that polaritons are mostly affected by disorder acting on the photon component, thus confirming existing studies on the influence of exciton disorder. The polariton localization length is estimated to be in the few-micrometres range, depending on the amplitude of disorder, in agreement with recent experimental findings

  7. Atomistic theory of excitonic fine structure in InAs/InP nanowire quantum dot molecules

    Science.gov (United States)

    Świderski, M.; Zieliński, M.

    2017-03-01

    Nanowire quantum dots have peculiar electronic and optical properties. In this work we use atomistic tight binding to study excitonic spectra of artificial molecules formed by a double nanowire quantum dot. We demonstrate a key role of atomistic symmetry and nanowire substrate orientation rather than cylindrical shape symmetry of a nanowire and a molecule. In particular for [001 ] nanowire orientation we observe a nonvanishing bright exciton splitting for a quasimolecule formed by two cylindrical quantum dots of different heights. This effect is due to interdot coupling that effectively reduces the overall symmetry, whereas single uncoupled [001 ] quantum dots have zero fine structure splitting. We found that the same double quantum dot system grown on [111 ] nanowire reveals no excitonic fine structure for all considered quantum dot distances and individual quantum dot heights. Further we demonstrate a pronounced, by several orders of magnitude, increase of the dark exciton optical activity in a quantum dot molecule as compared to a single quantum dot. For [111 ] systems we also show spontaneous localization of single particle states in one of nominally identical quantum dots forming a molecule, which is mediated by strain and origins from the lack of the vertical inversion symmetry in [111 ] nanostructures of overall C3 v symmetry. Finally, we study lowering of symmetry due to alloy randomness that triggers nonzero excitonic fine structure and the dark exciton optical activity in realistic nanowire quantum dot molecules of intermixed composition.

  8. Chromophore-Dependent Intramolecular Exciton-Vibrational Coupling in the FMO Complex: Quantification and Importance for Exciton Dynamics.

    Science.gov (United States)

    Padula, Daniele; Lee, Myeong H; Claridge, Kirsten; Troisi, Alessandro

    2017-11-02

    In this paper, we adopt an approach suitable for monitoring the time evolution of the intramolecular contribution to the spectral density of a set of identical chromophores embedded in their respective environments. We apply the proposed method to the Fenna-Matthews-Olson (FMO) complex, with the objective to quantify the differences among site-dependent spectral densities and the impact of such differences on the exciton dynamics of the system. Our approach takes advantage of the vertical gradient approximation to reduce the computational demands of the normal modes analysis. We show that the region of the spectral density that is believed to strongly influence the exciton dynamics changes significantly in the timescale of tens of nanoseconds. We then studied the impact of the intramolecular vibrations on the exciton dynamics by considering a model of FMO in a vibronic basis and neglecting the interaction with the environment to isolate the role of the intramolecular exciton-vibration coupling. In agreement with the assumptions in the literature, we demonstrate that high frequency modes at energy much larger than the excitonic energy splitting have negligible influence on exciton dynamics despite the large exciton-vibration coupling. We also find that the impact of including the site-dependent spectral densities on exciton dynamics is not very significant, indicating that it may be acceptable to apply the same spectral density on all sites. However, care needs to be taken for the description of the exciton-vibrational coupling in the low frequency part of intramolecular modes because exciton dynamics is more susceptible to low frequency modes despite their small Huang-Rhys factors.

  9. Time-resolved photon echoes from donor-bound excitons in ZnO epitaxial layers

    Science.gov (United States)

    Poltavtsev, S. V.; Kosarev, A. N.; Akimov, I. A.; Yakovlev, D. R.; Sadofev, S.; Puls, J.; Hoffmann, S. P.; Albert, M.; Meier, C.; Meier, T.; Bayer, M.

    2017-07-01

    The coherent optical response from 140 nm and 65 nm thick ZnO epitaxial layers is studied using four-wave-mixing spectroscopy with picosecond temporal resolution. Resonant excitation of neutral donor-bound excitons results in two-pulse and three-pulse photon echoes. For the donor-bound A exciton (D0XA ) at temperature of 1.8 K we evaluate optical coherence times T2=33 -50 ps corresponding to homogeneous line widths of 13 -19 μ eV , about two orders of magnitude smaller as compared with the inhomogeneous broadening of the optical transitions. The coherent dynamics is determined mainly by the population decay with time T1=30 -40 ps, while pure dephasing is negligible. Temperature increase leads to a significant shortening of T2 due to interaction with acoustic phonons. In contrast, the loss of coherence of the donor-bound B exciton (D0XB ) is significantly faster (T2=3.6 ps ) and governed by pure dephasing processes.

  10. Excitonic and electron-hole mechanisms of the creation of Frenkel defect in alkali halides

    International Nuclear Information System (INIS)

    Lushchik, A.; Kirm, M.; Lushchik, Ch.; Vasil'chenko, E.

    2000-01-01

    Excitonic and electron-hole (e-h) mechanisms of stable F centre creation by VUV radiation in alkali halide crystals are discussed. In KCl at 4.2 K, the efficiency of stable F-H pair creation is especially high at the direct optical formation of triplet excitons with n=1. At 200-400 K, the creation processes of stable F centres in KCl are especially efficient at the formation of one-halide exciton in the Urbach tail of an exciton absorption. In KCl and KBr, the decay of a cation exciton (∼20 eV) causes the formation of two e-h pairs, while in NaCl a cation exciton (33.5 eV) decays into two e-h and an anion exciton. An elastic uniaxial stress of a crystal excited by VUV radiation decreases the mean free path of excitons before their self-trapping (KI) and increases the mean free path of hot holes before self-trapping (NaCl)

  11. Nano-Optics: Coherent Nonlinear Optical Response and Control of Single Quantum Dots

    National Research Council Canada - National Science Library

    Steel, Duncan

    2002-01-01

    .... These features include optically induced and detected quantum entanglement of two exciton states as well as a demonstration of a classical Bell state, a Rabi oscillations corresponding to full...

  12. Ultrafast dynamics of Coulomb correlated excitons in GaAs quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Mycek, M.A. [Univ. of California, Berkeley, CA (United States). Dept. of Physics]|[Lawrence Berkeley National Lab., CA (United States). Materials Sciences Div.

    1995-12-01

    The author measures the transient nonlinear optical response of room temperature excitons in gallium arsenide quantum wells via multi-wave mixing experiments. The dynamics of the resonantly excited excitons is directly reflected by the ultrafast decay of the induced nonlinear polarization, which radiates the detected multi-wave mixing signal. She characterizes this ultrafast coherent emission in both amplitude and phase, using time- and frequency-domain measurement techniques, to better understand the role of Coulomb correlation in these systems. To interpret the experimental results, the nonlinear optical response of a dense medium is calculated using a model including Coulomb interaction. She contributes three new elements to previous theoretical and experimental studies of these systems. First, surpassing traditional time-integrated measurements, she temporally resolves the amplitude of the ultrafast coherent emission. Second, in addition to measuring the third-order four-wave mixing signal, she also investigates the fifth-order six-wave mixing response. Third, she characterizes the ultrafast phase dynamics of the nonlinear emission using interferometric techniques with an unprecedented resolution of approximately 140 attoseconds. The author finds that effects arising from Coulomb correlation dominate the nonlinear optical response when the density of excitons falls below 3 {times} 10{sup 11} cm{sup {minus}2}, the saturation density. These signatures of Coulomb correlation are investigated for increasing excitation density to gradually screen the interactions and test the validity of the model for dense media. The results are found to be qualitatively consistent with both the predictions of the model and with numerical solutions to the semiconductor Bloch equations. Importantly, the results also indicate current experimental and theoretical limitations, which should be addressed in future research.

  13. Effective-mass model and magneto-optical properties in hybrid perovskites

    OpenAIRE

    Yu, Z. G.

    2016-01-01

    Hybrid inorganic-organic perovskites have proven to be a revolutionary material for low-cost photovoltaic applications. They also exhibit many other interesting properties, including giant Rashba splitting, large-radius Wannier excitons, and novel magneto-optical effects. Understanding these properties as well as the detailed mechanism of photovoltaics requires a reliable and accessible electronic structure, on which models of transport, excitonic, and magneto-optical properties can be effici...

  14. Coherent dynamics of interwell excitons in GaAs/AlxGa1-xAs superlattices

    DEFF Research Database (Denmark)

    Mizeikis, V.; Birkedal, Dan; Langbein, Wolfgang Werner

    1997-01-01

    Coherent exciton dynamics in a GaAs/AlxGa1-xAs narrow-miniband superlattice is studied by spectrally resolved transient four-wave mixing. Coherent optical properties of the investigated structure are found to be strongly affected by the existence of two different heavy-hole excitonic states. One...

  15. Probing exciton density of states through phonon-assisted emission in GaN epilayers: A and B exciton contributions

    Science.gov (United States)

    Cavigli, Lucia; Gabrieli, Riccardo; Gurioli, Massimo; Bogani, Franco; Feltin, Eric; Carlin, Jean-François; Butté, Raphaël; Grandjean, Nicolas; Vinattieri, Anna

    2010-09-01

    A detailed experimental investigation of the phonon-assisted emission in a high-quality c -plane GaN epilayer is presented up to 200 K. By performing photoluminescence and reflectivity measurements, we find important etaloning effects in the phonon-replica spectra, which have to be corrected before addressing the lineshape analysis. Direct experimental evidence for free exciton thermalization is found for the whole temperature range investigated. A close comparison with existing models for phonon replicas originating from a thermalized free exciton distribution shows that the simplified and commonly adopted description of the exciton-phonon interaction with a single excitonic band leads to a large discrepancy with experimental data. Only the consideration of the complex nature of the excitonic band in GaN, including A and B exciton contributions, allows accounting for the temperature dependence of the peak energy, intensity, and lineshape of the phonon replicas.

  16. 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).

  17. Optical absorption of charged excitons in semiconducting carbon nanotubes

    DEFF Research Database (Denmark)

    Rønnow, Troels Frimodt; Pedersen, Thomas Garm; Cornean, Horia

    2012-01-01

    In this article we examine the absorption coefficient of charged excitons in carbon nanotubes. We investigate the temperature and damping dependence of the absorption spectra. We show that the trion peak in the spectrum is asymmetric for temperatures greater than approximately 1 K whereas...

  18. Theory of Excitonic Delocalization for Robust Vibronic Dynamics in LH2.

    Science.gov (United States)

    Caycedo-Soler, Felipe; Lim, James; Oviedo-Casado, Santiago; van Hulst, Niek F; Huelga, Susana F; Plenio, Martin B

    2018-06-11

    Nonlinear spectroscopy has revealed long-lasting oscillations in the optical response of a variety of photosynthetic complexes. Different theoretical models that involve the coherent coupling of electronic (excitonic) or electronic-vibrational (vibronic) degrees of freedom have been put forward to explain these observations. The ensuing debate concerning the relevance of either mechanism may have obscured their complementarity. To illustrate this balance, we quantify how the excitonic delocalization in the LH2 unit of Rhodopseudomonas acidophila purple bacterium leads to correlations of excitonic energy fluctuations, relevant coherent vibronic coupling, and importantly, a decrease in the excitonic dephasing rates. Combining these effects, we identify a feasible origin for the long-lasting oscillations observed in fluorescent traces from time-delayed two-pulse single-molecule experiments performed on this photosynthetic complex and use this approach to discuss the role of this complementarity in other photosynthetic systems.

  19. Wannier-Mott Excitons in Nanoscale Molecular Ices

    Science.gov (United States)

    Chen, Y.-J.; Muñoz Caro, G. M.; Aparicio, S.; Jiménez-Escobar, A.; Lasne, J.; Rosu-Finsen, A.; McCoustra, M. R. S.; Cassidy, A. M.; Field, D.

    2017-10-01

    The absorption of light to create Wannier-Mott excitons is a fundamental feature dictating the optical and photovoltaic properties of low band gap, high permittivity semiconductors. Such excitons, with an electron-hole separation an order of magnitude greater than lattice dimensions, are largely limited to these semiconductors but here we find evidence of Wannier-Mott exciton formation in solid carbon monoxide (CO) with a band gap of >8 eV and a low electrical permittivity. This is established through the observation that a change of a few degrees K in deposition temperature can shift the electronic absorption spectra of solid CO by several hundred wave numbers, coupled with the recent discovery that deposition of CO leads to the spontaneous formation of electric fields within the film. These so-called spontelectric fields, here approaching 4 ×107 V m-1 , are strongly temperature dependent. We find that a simple electrostatic model reproduces the observed temperature dependent spectral shifts based on the Stark effect on a hole and electron residing several nm apart, identifying the presence of Wannier-Mott excitons. The spontelectric effect in CO simultaneously explains the long-standing enigma of the sensitivity of vacuum ultraviolet spectra to the deposition temperature.

  20. Superposition of the luminescence spectra of free and bound excitons in ZnP2-D48

    International Nuclear Information System (INIS)

    Stamov, Ion; Nemerenco, Lucretia; Ivanenco, Iurii; Syrbu, Nicolae

    2011-01-01

    The luminescence spectra of ZnP 2 tetragonal crystals doped Mn, Sn, Cd, Sb at 10 K emission lines of bound excitons is detected. In the spectra non-phonon emission lines of bound and free excitons and their phonon replicas is isolated. The emission lines by the levels of the axial center are described. The composition of the luminescence of free and bound excitons at the axial center is investigated. In the region of phonon replicas of free excitons observed enhancement of lines due to forbidden transitions involving the recombination of excitons. A model of optic recombination transitions of the axial centre is proposed

  1. Tailoring double Fano profiles with plasmon-assisted quantum interference in hybrid exciton-plasmon system

    International Nuclear Information System (INIS)

    Zhao, Dongxing; Wu, Jiarui; Gu, Ying; Gong, Qihuang

    2014-01-01

    We propose tailoring of the double Fano profiles via plasmon-assisted quantum interference in a hybrid exciton-plasmon system. Tailoring is performed by the interference between two exciton channels interacting with a common localized surface plasmon. Using an applied field of low intensity, the absorption spectrum of the hybrid system reveals a double Fano lineshape with four peaks. For relatively large field intensity, a broad flat window in the absorption spectrum appears which results from the destructive interference between excitons. Because of strong constructive interference, this window vanishes as intensity is further increased. We have designed a nanometer bandpass optical filter for visible light based on tailoring of the optical spectrum. This study provides a platform for quantum interference that may have potential applications in ultracompact tunable quantum devices.

  2. Magneto-exciton transitions in laterally coupled quantum dots

    Science.gov (United States)

    Barticevic, Zdenka; Pacheco, Monica; Duque, Carlos A.; Oliveira, Luiz E.

    2008-03-01

    We present a study of the electronic and optical properties of laterally coupled quantum dots. The excitonic spectra of this system under the effects of an external magnetic field applied perpendicular to the plane of the dots is obtained, with the potential of every individual dot taken as the superposition of a quantum well potential along the axial direction with a lateral parabolic confinement potential, and the coupled two- dot system then modeled by a superposition of the potentials of each dot, with their minima at different positions and truncated at the intersection plane. The wave functions and eigenvalues are obtained in the effective-mass approximation by using an extended variational approach in which the magneto- exciton states are simultaneously obtained [1]. The allowed magneto-exciton transitions are investigated by using circularly polarized radiation in the plane perpendicular to the magnetic field. We present results on the excitonic absorption coefficient as a function of the photon energy for different geometric quantum-dot confinement and magnetic-field values. Reference: [1] Z. Barticevic, M. Pacheco, C. A. Duque and L. E. Oliveira, Phys. Rev. B 68, 073312 (2003).

  3. Wannier-Frenkel hybrid exciton in organic-semiconductor quantum dot heterostructures

    International Nuclear Information System (INIS)

    Birman, Joseph L.; Huong, Nguyen Que

    2007-01-01

    The formation of a hybridization state of Wannier Mott exciton and Frenkel exciton in different hetero-structure configurations involving quantum dots is investigated. The hybrid excitons exist at the interfaces of the semiconductors quantum dots and the organic medium, having unique properties and a large optical non-linearity. The coupling at resonance is very strong and tunable by changing the parameters of the systems (dot radius, dot-dot distance, generation of the organic dendrites and the materials of the system etc...). Different semiconductor quantum dot-organic material combination systems have been considered such as a semiconductor quantum dot lattice embedded in an organic host, a semiconductor quantum dot at the center of an organic dendrite, a semiconductor quantum dot coated by an organic shell

  4. Quantum confinement-induced tunable exciton states in graphene oxide.

    Science.gov (United States)

    Lee, Dongwook; Seo, Jiwon; Zhu, Xi; Lee, Jiyoul; Shin, Hyeon-Jin; Cole, Jacqueline M; Shin, Taeho; Lee, Jaichan; Lee, Hangil; Su, Haibin

    2013-01-01

    Graphene oxide has recently been considered to be a potential replacement for cadmium-based quantum dots due to its expected high fluorescence. Although previously reported, the origin of the luminescence in graphene oxide is still controversial. Here, we report the presence of core/valence excitons in graphene-based materials, a basic ingredient for optical devices, induced by quantum confinement. Electron confinement in the unreacted graphitic regions of graphene oxide was probed by high resolution X-ray absorption near edge structure spectroscopy and first-principles calculations. Using experiments and simulations, we were able to tune the core/valence exciton energy by manipulating the size of graphitic regions through the degree of oxidation. The binding energy of an exciton in highly oxidized graphene oxide is similar to that in organic electroluminescent materials. These results open the possibility of graphene oxide-based optoelectronic device technology.

  5. Robust tunable excitonic features in monolayer transition metal dichalcogenide quantum dots

    Science.gov (United States)

    Fouladi-Oskouei, J.; Shojaei, S.; Liu, Z.

    2018-04-01

    The effects of quantum confinement on excitons in parabolic quantum dots of monolayer transition metal dichalcogenides (TMDC QDs) are investigated within a massive Dirac fermion model. A giant spin-valley coupling of the TMDC QDs is obtained, larger than that of monolayer TMDC sheets and consistent with recent experimental measurements. The exciton transition energy and the binding energy are calculated, and it is found that the strong quantum confinement results in extremely high exciton binding energies. The enormously large exciton binding energy in TMDC QDs (({{E}{{B2D}}}∼ 500 meV)different kinds of TMDC QDs) ensures that the many body interactions play a significant role in the investigation of the optical properties of these novel nanostructures. The estimated oscillator strength and radiative lifetime of excitons are strongly size-dependent and indicate a giant oscillator strength enhancement and ultrafast radiative annihilation of excitons, varying from a few tens of femtoseconds to a few picoseconds. We found that the spin-dependent band gap, spin-valley coupling, binding energy and excitonic effects can be tuned by quantum confinements, leading to tunable quantum dots in monolayer TMDCs. This finding offers new functionality in engineering the interaction of a 2D material with light and creates promise for the quantum manipulation of spin and valley degrees of freedom in TMDC nanostructures, enabling versatile novel 2D quantum photonic and optoelectronic nanodevices.

  6. Phonon effects on the radiative recombination of excitons in double quantum dots

    Science.gov (United States)

    Karwat, Paweł; Sitek, Anna; Machnikowski, Paweł

    2011-11-01

    We study theoretically the radiative recombination of excitons in double quantum dots in the presence of carrier-phonon coupling. We show that the phonon-induced pure dephasing effects and transitions between the exciton states strongly modify the spontaneous emission process and make it sensitive to temperature, which may lead to nonmonotonic temperature dependence of the time-resolved luminescence. We show also that, under specific resonance conditions, the biexcitonic interband polarization can be coherently transferred to the excitonic one, leading to an extended lifetime of the total coherent polarization, which is reflected in the nonlinear optical spectrum of the system. We study the stability of this effect against phonon-induced decoherence.

  7. Features of exciton dynamics in molecular nanoclusters (J-aggregates): Exciton self-trapping (Review Article)

    Science.gov (United States)

    Malyukin, Yu. V.; Sorokin, A. V.; Semynozhenko, V. P.

    2016-06-01

    We present thoroughly analyzed experimental results that demonstrate the anomalous manifestation of the exciton self-trapping effect, which is already well-known in bulk crystals, in ordered molecular nanoclusters called J-aggregates. Weakly-coupled one-dimensional (1D) molecular chains are the main structural feature of J-aggregates, wherein the electron excitations are manifested as 1D Frenkel excitons. According to the continuum theory of Rashba-Toyozawa, J-aggregates can have only self-trapped excitons, because 1D excitons must adhere to barrier-free self-trapping at any exciton-phonon coupling constant g = ɛLR/2β, wherein ɛLR is the lattice relaxation energy, and 2β is the half-width of the exciton band. In contrast, very often only the luminescence of free, mobile excitons would manifest in experiments involving J-aggregates. Using the Urbach rule in order to analyze the low-frequency region of the low-temperature exciton absorption spectra has shown that J-aggregates can have both a weak (g 1) exciton-phonon coupling. Moreover, it is experimentally demonstrated that under certain conditions, the J-aggregate excited state can have both free and self-trapped excitons, i.e., we establish the existence of a self-trapping barrier for 1D Frenkel excitons. We demonstrate and analyze the reasons behind the anomalous existence of both free and self-trapped excitons in J-aggregates, and demonstrate how exciton-self trapping efficiency can be managed in J-aggregates by varying the values of g, which is fundamentally impossible in bulk crystals. We discuss how the exciton-self trapping phenomenon can be used as an alternate interpretation of the wide band emission of some J-aggregates, which has thus far been explained by the strongly localized exciton model.

  8. Exciton-polariton dynamics in a GaAs bulk microcavity

    Science.gov (United States)

    Ceccherini, S.; Gurioli, M.; Bogani, F.; Colocci, M.; Tredicucci, A.; Bassani, F.; Beltram, F.; Sorba, L.

    1998-01-01

    We present a full analysis of exciton dynamics in a GaAs λ/2 bulk microcavity following excitation by ultrafast laser pulses. Coherent dynamics was probed by means of an interferometric technique; beating and dephasing times were studied for various excitation intensities. At high incident power, population effects begin to show up reducing exciton oscillator strength and suppressing Rabi splitting. This feature produces marked non-linearities in the input-output characteristic of the optical functions, which were studied in view of reaching bistable operation. Theoretical calculations performed within the transfer-matrix framework show good agreement with experimental results.

  9. Perovskite Excitonics : Primary Exciton Creation and Crossover from Free Carriers to a Secondary Exciton Phase

    NARCIS (Netherlands)

    Sarritzu, Valerio; Sestu, Nicola; Marongiu, Daniela; Chang, Xueqing; Wang, Qingqian; Loi, Maria Antonietta; Quochi, Francesco; Saba, Michele; Mura, Andrea; Bongiovanni, Giovanni

    2018-01-01

    Understanding exciton formation is of fundamental importance for emerging optoelectronic materials, like hybrid organic-inorganic perovskites, as excitons are the lowest-energy photoexcitations in semiconductors, are electrically neutral, and do not directly contribute to charge transport, but can

  10. Spin-dependent exciton-exciton interaction potential in two- and three-dimensional structure semiconductors under excitation

    International Nuclear Information System (INIS)

    Nguyen Ba An; Hoang Ngoc Cam; Nguyen Trung Dan

    1990-08-01

    Analytical expressions of the exciton-exciton interaction potentials have been approximately derived in both 2D and 3D structure materials exhibiting explicit dependences on exciton momentum difference, momentum transfer, electron-hole effective mass ratio and two-exciton state spin symmetry. Numerical calculations show that the character of the exciton-exciton interaction is determined by all of the above-mentioned dependences. (author). 32 refs, 7 figs

  11. Excitonic Behavior of Rhodamine Dimers: A Single-Molecule Study

    NARCIS (Netherlands)

    Hernando Campos, J.; van der Schaaf, Martijn; van Dijk, E.M.H.P.; Sauer, Markus; Garcia Parajo, M.F.; van Hulst, N.F.

    2003-01-01

    The optical behavior of a dimer of tetramethylrhodamine-5-isothiocyanate has been investigated by means of single-molecule measurements. Bulk absorption and fluorescence spectra show the existence of two populations of the dimer molecule that exhibit distinct excitonic interactions (strong and weak

  12. Surface Plasmon Polariton-Assisted Long-Range Exciton Transport in Monolayer Semiconductor Lateral Heterostructure

    Science.gov (United States)

    Shi, Jinwei; Lin, Meng-Hsien; Chen, Yi-Tong; Estakhri, Nasim Mohammadi; Tseng, Guo-Wei; Wang, Yanrong; Chen, Hung-Ying; Chen, Chun-An; Shih, Chih-Kang; Alã¹, Andrea; Li, Xiaoqin; Lee, Yi-Hsien; Gwo, Shangjr

    Recently, two-dimensional (2D) semiconductor heterostructures, i.e., atomically thin lateral heterostructures (LHSs) based on transition metal dichalcogenides (TMDs) have been demonstrated. In an optically excited LHS, exciton transport is typically limited to a rather short spatial range ( 1 micron). Furthermore, additional losses may occur at the lateral interfacial regions. Here, to overcome these challenges, we experimentally implement a planar metal-oxide-semiconductor (MOS) structure by placing a monolayer of WS2/MoS2 LHS on top of an Al2O3 capped Ag single-crystalline plate. We found that the exciton transport range can be extended to tens of microns. The process of long-range exciton transport in the MOS structure is confirmed to be mediated by an exciton-surface plasmon polariton-exciton conversion mechanism, which allows a cascaded energy transfer process. Thus, the planar MOS structure provides a platform seamlessly combining 2D light-emitting materials with plasmonic planar waveguides, offering great potential for developing integrated photonic/plasmonic functionalities.

  13. Colloquium: Excitons in atomically thin transition metal dichalcogenides

    Science.gov (United States)

    Wang, Gang; Chernikov, Alexey; Glazov, Mikhail M.; Heinz, Tony F.; Marie, Xavier; Amand, Thierry; Urbaszek, Bernhard

    2018-04-01

    Atomically thin materials such as graphene and monolayer transition metal dichalcogenides (TMDs) exhibit remarkable physical properties resulting from their reduced dimensionality and crystal symmetry. The family of semiconducting transition metal dichalcogenides is an especially promising platform for fundamental studies of two-dimensional (2D) systems, with potential applications in optoelectronics and valleytronics due to their direct band gap in the monolayer limit and highly efficient light-matter coupling. A crystal lattice with broken inversion symmetry combined with strong spin-orbit interactions leads to a unique combination of the spin and valley degrees of freedom. In addition, the 2D character of the monolayers and weak dielectric screening from the environment yield a significant enhancement of the Coulomb interaction. The resulting formation of bound electron-hole pairs, or excitons, dominates the optical and spin properties of the material. Here recent progress in understanding of the excitonic properties in monolayer TMDs is reviewed and future challenges are laid out. Discussed are the consequences of the strong direct and exchange Coulomb interaction, exciton light-matter coupling, and influence of finite carrier and electron-hole pair densities on the exciton properties in TMDs. Finally, the impact on valley polarization is described and the tuning of the energies and polarization observed in applied electric and magnetic fields is summarized.

  14. Fermi-edge exciton-polaritons in doped semiconductor microcavities with finite hole mass

    Science.gov (United States)

    Pimenov, Dimitri; von Delft, Jan; Glazman, Leonid; Goldstein, Moshe

    2017-10-01

    The coupling between a 2D semiconductor quantum well and an optical cavity gives rise to combined light-matter excitations, the exciton-polaritons. These were usually measured when the conduction band is empty, making the single polariton physics a simple single-body problem. The situation is dramatically different in the presence of a finite conduction-band population, where the creation or annihilation of a single exciton involves a many-body shakeup of the Fermi sea. Recent experiments in this regime revealed a strong modification of the exciton-polariton spectrum. Previous theoretical studies concerned with nonzero Fermi energy mostly relied on the approximation of an immobile valence-band hole with infinite mass, which is appropriate for low-mobility samples only; for high-mobility samples, one needs to consider a mobile hole with large but finite mass. To bridge this gap, we present an analytical diagrammatic approach and tackle a model with short-ranged (screened) electron-hole interaction, studying it in two complementary regimes. We find that the finite hole mass has opposite effects on the exciton-polariton spectra in the two regimes: in the first, where the Fermi energy is much smaller than the exciton binding energy, excitonic features are enhanced by the finite mass. In the second regime, where the Fermi energy is much larger than the exciton binding energy, finite mass effects cut off the excitonic features in the polariton spectra, in qualitative agreement with recent experiments.

  15. Bistable behaviour of biexciton population in a dense exciton-biexciton system in semiconductors

    International Nuclear Information System (INIS)

    Nguyen Ba An.

    1986-05-01

    The steady state bistable behaviour of biexciton population in a dense exciton-biexciton semiconductor is considered. The intrinsic optical feedback is provided by the recombination mechanism. The exciton-biexciton and biexciton-biexciton interactions play the role of non-linearity responsible for biexciton bistability to occur. The conditions leading to the effect of bistability are obtained and two-parameter phase transition diagrams are drawn for both intensity and frequency bistable phenomena. (author)

  16. On the equivalence of two approaches in the exciton-polariton theory

    International Nuclear Information System (INIS)

    Ha Vinh Tan; Nguyen Toan Thang

    1983-02-01

    The polariton effect in the optical processes involving photons with energies near that of an exciton is investigated by the Bogolubov diagonalization and the Green function approaches in a simple model of the direct band gap semiconductor with the electrical dipole allowed transition. To take into account the non-resonant terms of the interaction Hamiltonian of the photon-exciton system the Green function approach derived by Nguyen Van Hieu is presented with the use of Green's function matrix technique analogous to that suggested by Nambu in the theory of superconductivity. It is shown that with the suitable choice of the phase factors the renormalization constants are equal to the diagonalization coefficients. The disperson of polaritons and the matrix elements of processes with the participation of polaritons are identically calculated by both methods. However the Green function approach has an advantage in including the damping effect of polaritons. (author)

  17. Frenkel-Charge-Transfer exciton intermixing theory for molecular crystals with two isolated Frenkel exciton states.

    Science.gov (United States)

    Bondarev, Igor; Popescu, Adrian

    We develop an analytical theory for the intra-intermolecular exciton intermixing in periodic 1D chains of planar organic molecules with two isolated low-lying Frenkel exciton states, typical of copper phthalocyanine (CuPc) and other transition metal phthalocyanine molecules. We formulate the Hamiltonian and use the exact Bogoliubov diagonalization procedure to derive the eigen energy spectrum for the two lowest intramolecular Frenkel excitons coupled to the intermolecular charge transfer (CT) exciton state. By comparing our theoretical spectrum with available experimental CuPc absorption data, we obtain the parameters of the Frenkel-CT exciton intermixing in CuPc thin films. The two Frenkel exciton states here are spaced apart by 0.26 eV, and the charge transfer exciton state is 50 meV above the lowest Frenkel exciton. Both Frenkel excitons are strongly mixed with the CT exciton, showing the coupling constant 0.17 eV in agreement with earlier electron transport experiments. Our results can be used for the proper interpretation of the physical properties of crystalline phthalocyanines. DOE-DE-SC0007117 (I.B.), UNC-GA ROI Grant (A.P.).

  18. Mapping the nanoscale energetic landscape in conductive polymer films with spatially super-resolved exciton dynamics

    Science.gov (United States)

    Ginsberg, Naomi

    2015-03-01

    The migration of Frenkel excitons, tightly-bound electron-hole pairs, in polymeric organic semiconducting films is critical to the efficiency of bulk heterojunction solar cells. While these materials exhibit a high degree of structural heterogeneity on the nanoscale, traditional measurements of exciton diffusion lengths are performed on bulk samples. Since both the characteristic length scales of structural heterogeneity and the reported bulk diffusion lengths are smaller than the optical diffraction limit, we adapt far-field super-resolution fluorescence imaging to uncover the correlations between the structural and energetic landscapes that the excitons explore.

  19. Optical techniques for probing the excited state dynamics of quantum dot solids

    Energy Technology Data Exchange (ETDEWEB)

    Moroz, P.; Kholmicheva, N.; Razgoniaeva, N. [Center for Photochemical Sciences, Bowling Green State University, Bowling Green, OH 43402 (United States); Department of Physics, Bowling Green State University, Bowling Green, OH 43402 (United States); Burchfield, D. [Department of Chemistry, Bowling Green State University, Bowling Green, OH 43402 (United States); Sharma, N.; Acharya, A. [Department of Physics, Bowling Green State University, Bowling Green, OH 43402 (United States); Zamkov, M., E-mail: zamkovm@bgsu.edu [Center for Photochemical Sciences, Bowling Green State University, Bowling Green, OH 43402 (United States); Department of Physics, Bowling Green State University, Bowling Green, OH 43402 (United States)

    2016-06-01

    Highlights: • Optical techniques represent a powerful tool for probing exciton diffusion in QD solids. • Exciton dissociation in QD solids is caused by charge tunneling to traps and other dots. • Exciton and free-carrier lifetimes are given by fast and slow components of PL decay. • Surface PL offers valuable information on the type and density of traps in QD solids. - Abstract: Quantum dot (QD) solids represent an important class of functional materials that holds strong promise for future applications in technology. Their optoelectronic properties are determined by energy diffusion processes, which character can often be inferred from the temporal and spectral analysis of the film’s photoluminescence (PL). Here, optical techniques based on PL lifetime, bulk quenching, and temperature-dependent PL will be discussed. These techniques complement the electrical conductivity measurements by mapping the flow of optically induced excitons through undepleted, contact-free films with an unprecedented temporal and spatial resolution. By correlating the QD solid morphology with the ensuing photoluminescence (PL) dynamics, these methods allow estimating important transport characteristics, including exciton and charge carrier diffusion lengths, the rate of interparticle energy transfer, carrier mobility, and the exciton diffusivity. The review will cover most popular PL-based strategies and summarize the key experimental findings resulting from these works.

  20. Exciton Recombination in Formamidinium Lead Triiodide : Nanocrystals versus Thin Films

    NARCIS (Netherlands)

    Fang, Hong-Hua; Protesescu, Loredana; Balazs, Daniel M.; Adjokatse, Sampson; Kovalenko, Maksym V.; Loi, Maria Antonietta

    2017-01-01

    The optical properties of the newly developed near-infrared emitting formamidinium lead triiodide (FAPbI(3)) nanocrystals (NCs) and their polycrystalline thin film counterpart are comparatively investigated by means of steady-state and time-resolved photoluminescence. The excitonic emission is

  1. The interplay between excitons and trions in a monolayer of MoSe2

    Science.gov (United States)

    Lundt, N.; Cherotchenko, E.; Iff, O.; Fan, X.; Shen, Y.; Bigenwald, P.; Kavokin, A. V.; Höfling, S.; Schneider, C.

    2018-01-01

    The luminescence and absorption properties of transition metal dichalcogenide monolayers are widely determined by neutral and charged excitonic complexes. Here, we focus on the impact of a free carrier reservoir on the optical properties of excitonic and trionic complexes in a MoSe2 monolayer at cryogenic temperatures. By applying photodoping via a non-resonant pump laser, the electron density can be controlled in our sample, which is directly reflected in the contribution of excitons and trions to the luminescence signal. We find significant shifts of both the exciton and trion energies in the presence of an induced electron gas both in power- and in time evolution (on the second to minute scale) in our photoluminescence spectra. In particular, in the presence of the photo-doped carrier reservoir, we observe that the splitting between excitons and trions can be enhanced by up to 4 meV. This behaviour is phenomenologically explained by an interplay between an increased screening of excitons via electrons in our system and a modification of the Fermi level. We introduce a simple but still quantitative treatment of these effects within a variational approach that takes into account both screening and phase space filling effects.

  2. Particle-in-a-box model of exciton absorption and electroabsorption in conjugated polymers

    Science.gov (United States)

    Pedersen, Thomas G.

    2000-12-01

    The recently proposed particle-in-a-box model of one-dimensional excitons in conjugated polymers is applied in calculations of optical absorption and electroabsorption spectra. It is demonstrated that for polymers of long conjugation length a superposition of single exciton resonances produces a line shape characterized by a square-root singularity in agreement with experimental spectra near the absorption edge. The effects of finite conjugation length on both absorption and electroabsorption spectra are analyzed.

  3. Electrical control of optical orientation of neutral and negatively charged excitons in an n -type semiconductor quantum well

    Science.gov (United States)

    Dzhioev, R. I.; Korenev, V. L.; Lazarev, M. V.; Sapega, V. F.; Gammon, D.; Bracker, A. S.

    2007-01-01

    We report electric field induced increase of spin orientation of negatively charged excitons (trions) localized in n -type GaAs/AlGaAs quantum well. Under resonant excitation of free neutral heavy-hole excitons, the polarization of trions increases dramatically with electrical injection of electrons. The polarization enhancement correlates strongly with trion/exciton luminescence intensity ratio. This effect results from a very efficient trapping of free neutral excitons by the quantum well interfacial fluctuations (“natural” quantum dots) containing resident electrons.

  4. Controlling the exciton energy of a nanowire quantum dot by strain fields

    Energy Technology Data Exchange (ETDEWEB)

    Chen, Yan; Zhang, Jiaxiang; Ding, Fei, E-mail: f.ding@ifw-dresden.de [Institute for Integrative Nanosciences, IFW Dresden, Helmholtz Strasse 20, 01069 Dresden (Germany); Zadeh, Iman Esmaeil; Jöns, Klaus D.; Fognini, Andreas; Zwiller, Val [Kavli Institute of Nanoscience, Delft University of Technology, 2600 GA Delft (Netherlands); Reimer, Michael E. [Institute for Quantum Computing and Department of Electrical and Computer Engineering, University of Waterloo, Waterloo, N2L 3G1 (Canada); Dalacu, Dan; Poole, Philip J. [National Research Council, Ottawa, Ontario K1A 0R6 (Canada); Schmidt, Oliver G. [Institute for Integrative Nanosciences, IFW Dresden, Helmholtz Strasse 20, 01069 Dresden (Germany); Material Systems for Nanoelectronics, Chemnitz University of Technology, Reichenhainer Strasse 70, 09107 Chemnitz (Germany)

    2016-05-02

    We present an experimental route to engineer the exciton energies of single quantum dots in nanowires. By integrating the nanowires onto a piezoelectric crystal, we controllably apply strain fields to the nanowire quantum dots. Consequently, the exciton energy of a single quantum dot in the nanowire is shifted by several meVs without degrading its optical intensity and single-photon purity. Second-order autocorrelation measurements are performed at different strain fields on the same nanowire quantum dot. The suppressed multi-photon events at zero time delay clearly verify that the quantum nature of single-photon emission is well preserved under external strain fields. The work presented here could facilitate on-chip optical quantum information processing with the nanowire based single photon emitters.

  5. Bistable Topological Insulator with Exciton-Polaritons

    Science.gov (United States)

    Kartashov, Yaroslav V.; Skryabin, Dmitry V.

    2017-12-01

    The functionality of many nonlinear and quantum optical devices relies on the effect of optical bistability. Using microcavity exciton-polaritons in a honeycomb arrangement of microcavity pillars, we report the resonance response and bistability of topological edge states. A balance between the pump, loss, and nonlinearity ensures a broad range of dynamical stability and controls the distribution of power between counterpropagating states on the opposite edges of the honeycomb lattice stripe. Tuning energy and polarization of the pump photons, while keeping their momentum constant, we demonstrate control of the propagation direction of the dominant edge state. Our results facilitate the development of practical applications of topological photonics.

  6. Excitonic dynamical Franz-Keldysh effect

    DEFF Research Database (Denmark)

    Nordstrøm, K.B.; Johnsen, Kristinn; Allen, S.J.

    1998-01-01

    The dynamical Franz-Keldysh effect is exposed by exploring near-band-gap absorption in the presence of intense THz electric fields. It bridges the gap between the de Franz-Keldysh effect and multiphoton absorption and competes with the THz ac Stark effect in shifting the energy of the excitonic...... resonance. A theoretical model which includes the strong THz field nonperturbatively via a nonequilibrium Green functions technique is able to describe the dynamical Franz-Keldysh effect in the presence of excitonic absorption....

  7. Optical Two-Dimensional Spectroscopy of Disordered Semiconductor Quantum Wells and Quantum Dots

    Energy Technology Data Exchange (ETDEWEB)

    Cundiff, Steven T. [Univ. of Colorado, Boulder, CO (United States)

    2016-05-03

    This final report describes the activities undertaken under grant "Optical Two-Dimensional Spectroscopy of Disordered Semiconductor Quantum Wells and Quantum Dots". The goal of this program was to implement optical 2-dimensional Fourier transform spectroscopy and apply it to electronic excitations, including excitons, in semiconductors. Specifically of interest are quantum wells that exhibit disorder due to well width fluctuations and quantum dots. In both cases, 2-D spectroscopy will provide information regarding coupling among excitonic localization sites.

  8. Strong exciton-photon coupling in organic single crystal microcavity with high molecular orientation

    Energy Technology Data Exchange (ETDEWEB)

    Goto, Kaname [Department of Electronics, Graduate School of Science and Technology, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585 (Japan); Yamashita, Kenichi, E-mail: yamasita@kit.ac.jp [Faculty of Electrical Engineering and Electronics, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585 (Japan); Yanagi, Hisao [Graduate School of Materials Science, Nara Institute of Science and Technology (NAIST), 8916-5 Takayama, Ikoma, Nara 630-0192 (Japan); Yamao, Takeshi; Hotta, Shu [Faculty of Materials Science and Technology, Kyoto Institute of Technology, Matsugasaki, Sakyo-ku, Kyoto 606-8585 (Japan)

    2016-08-08

    Strong exciton-photon coupling has been observed in a highly oriented organic single crystal microcavity. This microcavity consists of a thiophene/phenylene co-oligomer (TPCO) single crystal laminated on a high-reflection distributed Bragg reflector. In the TPCO crystal, molecular transition dipole was strongly polarized along a certain horizontal directions with respect to the main crystal plane. This dipole polarization causes significantly large anisotropies in the exciton transition and optical constants. Especially the anisotropic exciton transition was found to provide the strong enhancement in the coupling with the cavity mode, which was demonstrated by a Rabi splitting energy as large as ∼100 meV even in the “half-vertical cavity surface emitting lasing” microcavity structure.

  9. Strong exciton-photon coupling in organic single crystal microcavity with high molecular orientation

    Science.gov (United States)

    Goto, Kaname; Yamashita, Kenichi; Yanagi, Hisao; Yamao, Takeshi; Hotta, Shu

    2016-08-01

    Strong exciton-photon coupling has been observed in a highly oriented organic single crystal microcavity. This microcavity consists of a thiophene/phenylene co-oligomer (TPCO) single crystal laminated on a high-reflection distributed Bragg reflector. In the TPCO crystal, molecular transition dipole was strongly polarized along a certain horizontal directions with respect to the main crystal plane. This dipole polarization causes significantly large anisotropies in the exciton transition and optical constants. Especially the anisotropic exciton transition was found to provide the strong enhancement in the coupling with the cavity mode, which was demonstrated by a Rabi splitting energy as large as ˜100 meV even in the "half-vertical cavity surface emitting lasing" microcavity structure.

  10. Strong exciton-photon coupling in organic single crystal microcavity with high molecular orientation

    International Nuclear Information System (INIS)

    Goto, Kaname; Yamashita, Kenichi; Yanagi, Hisao; Yamao, Takeshi; Hotta, Shu

    2016-01-01

    Strong exciton-photon coupling has been observed in a highly oriented organic single crystal microcavity. This microcavity consists of a thiophene/phenylene co-oligomer (TPCO) single crystal laminated on a high-reflection distributed Bragg reflector. In the TPCO crystal, molecular transition dipole was strongly polarized along a certain horizontal directions with respect to the main crystal plane. This dipole polarization causes significantly large anisotropies in the exciton transition and optical constants. Especially the anisotropic exciton transition was found to provide the strong enhancement in the coupling with the cavity mode, which was demonstrated by a Rabi splitting energy as large as ∼100 meV even in the “half-vertical cavity surface emitting lasing” microcavity structure.

  11. Optical spectroscopy and system–bath interactions in molecular aggregates with full configuration interaction Frenkel exciton model

    Energy Technology Data Exchange (ETDEWEB)

    Seibt, Joachim; Sláma, Vladislav; Mančal, Tomáš, E-mail: mancal@karlov.mff.cuni.cz

    2016-12-20

    Highlights: • Standard Frenkel exciton model is extended to include inter-band coupling. • It is formally linked with configuration interaction method of quantum chemistry. • Spectral shifts due to inter-band coupling are found in molecular aggregates. • Effects of peak amplitude redistribution in two-dimensional spectra are found. - Abstract: Standard application of the Frenkel exciton model neglects resonance coupling between collective molecular aggregate states with different number of excitations. These inter-band coupling terms are, however, of the same magnitude as the intra-band coupling between singly excited states. We systematically derive the Frenkel exciton model from quantum chemical considerations, and identify it as a variant of the configuration interaction method. We discuss all non-negligible couplings between collective aggregate states, and provide compact formulae for their calculation. We calculate absorption spectra of molecular aggregate of carotenoids and identify significant band shifts as a result of inter-band coupling. The presence of inter-band coupling terms requires renormalization of the system–bath coupling with respect to standard formulation, but renormalization effects are found to be weak. We present detailed discussion of molecular dimer and calculate its time-resolved two-dimensional Fourier transformed spectra to find weak but noticeable effects of peak amplitude redistribution due to inter-band coupling.

  12. Nonlinear spectroscopy of excitons and biexcitons in ZnS

    International Nuclear Information System (INIS)

    Pavlov, L.I.; Paskov, P.P.; Lalov, I.J.

    1989-01-01

    Four- photon spectroscopy on exciton and biexciton states in ZnS is reported at T = 10 K. The Nd:YAG laser is used as a fundamental source in the experimental setup. Second harmonic radiation ω 2 pumps the dye laser of ω 1 tunable frequency. The ZnS single crystal is placed in an optical cryostat for resonant spectroscopy at low temperature. Four-photon mixing ω 3 = 2ω 1 -ω 2 signal is separated by MDR-23 monochromator and is registered by a laser photometer. The hexagonal ZnS crystal is experimentally investigated when the waves ω 1 and ω 2 propagate colinear with the optical axis. The crystal is cut along the (1120) plane. The photon 2ℎω 1 energy scans over the range 3.895-3.940 eV. The dispersion of I 3 (ω 3 ) upon 2ℎω 1 is obtained. Three resonances are registered E M = 3.8964, E B 1 = 3.9010 and E B 2 = 3.9311 eV. The recorded low temperature resonance in dispersion of nonlinearity χ (3) are identified with B 1 s and B 2 s excitons as well as with biexciton in ZnS which is observed for the first time in this crystal. An experimental dependence of the signal I 3 (ω 3 ) intensity upon the pump I 1 (ω 1 ) is obtained. The E M resonance is saturated with the I 1 (ω 1 ) enhancement while the E B 1 resonance increases. Authors explain such a behaviour by the fact that the recombination probability of the biexcitons to excitons increases with the pump level growth. Estimations for the exciton density and the bounding energy are given. (author)

  13. Real-Time Observation of Exciton-Phonon Coupling Dynamics in Self-Assembled Hybrid Perovskite Quantum Wells.

    Science.gov (United States)

    Ni, Limeng; Huynh, Uyen; Cheminal, Alexandre; Thomas, Tudor H; Shivanna, Ravichandran; Hinrichsen, Ture F; Ahmad, Shahab; Sadhanala, Aditya; Rao, Akshay

    2017-11-28

    Self-assembled hybrid perovskite quantum wells have attracted attention due to their tunable emission properties, ease of fabrication, and device integration. However, the dynamics of excitons in these materials, especially how they couple to phonons, remains an open question. Here, we investigate two widely used materials, namely, butylammonium lead iodide (CH 3 (CH 2 ) 3 NH 3 ) 2 PbI 4 and hexylammonium lead iodide (CH 3 (CH 2 ) 5 NH 3 ) 2 PbI 4 , both of which exhibit broad photoluminescence tails at room temperature. We performed femtosecond vibrational spectroscopy to obtain a real-time picture of the exciton-phonon interaction and directly identified the vibrational modes that couple to excitons. We show that the choice of the organic cation controls which vibrational modes the exciton couples to. In butylammonium lead iodide, excitons dominantly couple to a 100 cm -1 phonon mode, whereas in hexylammonium lead iodide, excitons interact with phonons with frequencies of 88 and 137 cm -1 . Using the determined optical phonon energies, we analyzed photoluminescence broadening mechanisms. At low temperatures (photoluminescence line shape observed in hybrid perovskite quantum wells and provide insights into the mechanism of exciton-phonon coupling in these materials.

  14. Terahertz field-induced ionization and perturbed free induction decay of excitons in bulk GaAs

    Science.gov (United States)

    Murotani, Yuta; Takayama, Masayuki; Sekiguchi, Fumiya; Kim, Changsu; Akiyama, Hidefumi; Shimano, Ryo

    2018-03-01

    We investigated the interaction between an intense terahertz (THz) pulse and excitons in bulk GaAs by using THz pump near-infrared (NIR) optical probe spectroscopy. We observed a clear spectral oscillation in the NIR transient absorption spectra at low temperature, which is interpreted as the THz pump-induced perturbed free induction decay (PFID) of the excitonic interband polarization. We performed a numerical simulation based on a microscopic theory and identified that the observed PFID signal originates from the THz field-induced ionization of excitons. Using a real-space representation of the excitonic wave function, we visualized how the ionization of an exciton proceeds under the intense single-cycle THz electric field. We also calculated the nonlinear susceptibility with the lowest-order perturbation theory assuming a weak THz pump, which showed a similar spectral feature with that obtained by the full treatment to field-induced ionization process. This coincidence is attributed to the fact that 1s-excitonic interband polarization is modified predominantly through interactions with the p-wave component of the excitonic wave function. A simple phenomenological expression of the PFID signal is presented to discuss effects of the THz pump pulse duration on the spectral oscillation.

  15. Effect of the dielectric constant of mesoscopic particle on the exciton binding energy

    International Nuclear Information System (INIS)

    Lai Zuyou; Gu Shiwei

    1991-09-01

    For materials with big exciton reduced mass and big dielectric constant, such as TiO 2 , the variation of dielectric constant with the radius of an ultrafine particle (UFP) is important for determining the exciton binding energy. For the first time a phenomenological formula of the dielectric constant of a UFP with its radius in mesoscopic range is put forward in order to explain the optical properties of TiO 2 UFP. (author). 22 refs, 3 figs, 1 tab

  16. Exploring ultrafast dynamics of excitons and multiexcitons in "giant" nanocrystal quantum dots

    Science.gov (United States)

    Sampat, Siddharth

    In this work, we have performed extensive time resolved photoluminescence (PL) studies to further the understanding of charge dynamics in semiconductor nanocrystal quantum dots (QDs). Recent developments in QD synthesis have introduced a new set of QD known as "giant" quantum dots (gQDs) that consist of a CdSe core coated with up to 19 monolayers of a CdS shell. The thick shell layer is grown using a SILAR method resulting in a defect free, alloyed CdSe/CdS interface. This has been attributed to gQDs exhibiting excellent optical properties such as high excitonic quantum yield (QY), prolonged photostability and inhibition of flourescence intermittency ("blinking"), which is regularly observed in conventional QDs. In gQDs, however, owing to unique fabrication methods and material selection, the Auger process is strongly suppressed resulting in efficient radiative recombination of photogenerated excitons as well as high PL QY of charged excitonic and multiexcitonic species. We perform extensive single gQDs studies that establish the role played by gQD shell thickness and core size in governing their optical properties. It is found that both the core and shell dimensions can be tuned in order to achieve the smallest gQDs with the highest vii Auger suppression resulting in photostable dots with high QYs. Next, we perform a study of multiexcitonic species in gQDs that are encapsulated in an insulating SiO2shell. These silica-coated gQDs exhibit strong PL from charged excitons, biexcitons as well as triexcitons. This observation has led to an accurate description of excitonic and multiexcitonic behavior which is modeled using a statistical scaling approach. As a demonstration of the practical applicability of gQDs, energy transfer of excitons as well as multiexcitons to different substrates is studied. Finally, a back gated silicon nanomembrane FET device is discussed that exhibits a large photocurrent increase when sensitized with QDs.

  17. Neutron scattering on equilibrium and nonequilibrium phonons, excitons and polaritons

    International Nuclear Information System (INIS)

    Broude, V.L.; Sheka, E.F.

    1978-01-01

    A number of problems of solid-state physics representing interest for neutron spectroscopy of future is considered. The development of the neutron inelastic scattering spectroscopy (neutron spectroscopy of equilibrium phonons) is discussed with application to nuclear dynamics of crystals in the thermodynamic equilibrium. The results of high-flux neutron source experiments on molecular crystals are presented. The advantages of neutron inelastic scattering over optical spectroscopy are discussed. The spectroscopy of quasi-equilibrium and non-equilibrium quasi-particles is discussed. In particular, the neutron scattering on polaritons, excitons in thermal equilibrium and production of light-excitons are considered. The problem of the possibility of such experiments is elucidated

  18. Exciton-polariton dynamics in quantum dot-cavity system

    Energy Technology Data Exchange (ETDEWEB)

    Neto, Antonio F.; Lima, William J.; Villas-Boas, Jose M. [Universidade Federal de Uberlandia (UFU), MG (Brazil). Inst. de Fisica

    2012-07-01

    Full text: One of the basic requirement for quantum information processing systems is the ability to completely control the state of a single qubit. This imply in know all sources of decoherence and elaborate ways to avoid them. In recent work, A. Laucht et al. [1] presented detailed theoretical and experimental investigations of electrically tunable single quantum dot (QD) - photonic crystal (PhC) nanocavity systems operating in the strong coupling regime of the light matter interaction. Unlike previous studies, where the exciton-cavity spectral detuning was varied by changing the lattice temperature, or by the adsorption of inert gases at low temperatures, they employ the quantum confined Stark-effect to electro-optically control the exciton-cavity detuning. The new built device enabled them to systematically probe the emission spectrum of the strongly coupled system as a function of external control parameters, as for example the incoherent excitation power density or the lattice temperature. Those studies reveal for the first time insights in dephasing mechanisms of 0D exciton polaritons [1]. In another study [2], using a similar device, they investigate the coupling between two different QDs with a single cavity mode. In both works, incoherent pumping was used, but for quantum information, coherent and controlled excitations are necessary. Here, we theoretically investigate the dynamics a single quantum dot inside a cavity under coherent pulse excitation and explore a wide range of parameters, as for example, the exciton-cavity detunings, the excitation power, the spontaneous decay, and pure dephasing. We use density matrix formalism in the Lindblad form, and we solve it numerically. Our results show that coherent excitation can be used to probe strong coupling between exciton and cavity mode by monitoring the exciton Rabi oscillation as function of the cavity detuning. This can give new insights for future experimental measurement focusing on quantum

  19. Energetic disorder and exciton states of individual molecular rings

    International Nuclear Information System (INIS)

    Herman, Pavel; Barvik, Ivan; Zapletal, David

    2006-01-01

    Exciton states in molecular rings (resembling, e.g. the B850 ring from LH2 complexes of purple bacterium Rhodopseudomonas acidophila) with strong intermolecular interaction are still a question of interest [V. Sundstrom, T. Pullerits, R. van Grondelle, J. Phys. Chem. B 103 (1999) 2327]. In our theoretical model we use the ring of two-level systems, simulating, e.g., the bacteriochlorophylls B850. The dynamical aspects in ensemble of rings are reflected in optical line shapes of electronic transitions. The observed linewidths reflect the combined influence of different types of static and dynamic disorder. To avoid the broadening of lines due to ensemble averaging one uses the single-molecule spectroscopy technique to obtain a fluorescence-excitation spectrum. For zero disorder the exciton manifold features two non-degenerate and eight pairwise degenerate states. In the presence of energetic disorder the degeneracy of the exciton states is lifted and oscillator strength is redistributed among the exciton states. A satisfactory understanding of the nature of static disorder in light-harvesting systems has not been reached [S. Jang, S.F. Dempster, R.J. Silbey, J. Phys. Chem. B 105 (2001) 6655]. In the local site basis, there can be present static disorder in both diagonal and off-diagonal Hamiltonian matrix elements. Silbey et al. [J. Phys. Chem. B 105 (2001) 6655] pointed out several questions: is former enough or the latter should be included as well? If both are considered, then there remains a question about whether they are independent or correlated. The distribution of the energetic separation E(k=+/-1) and relative orientation of the transition-dipole moments has been recently investigated [S. Jang, et al., J. Phys. Chem. B 105 (2001) 6655; C. Hofmann, T.J. Aartsma, J. Koehler, Chem. Phys. Lett. 395 (2004) 373]. In our present contribution we have extended such a type of investigation to four models of noncorrelated static disorder: (A) Gaussian disorder in the

  20. Pressure-Dependent Light Emission of Charged and Neutral Excitons in Monolayer MoSe 2

    Energy Technology Data Exchange (ETDEWEB)

    Fu, Xinpeng [State; Li, Fangfei [State; Lin, Jung-Fu [Department; Gong, Yuanbo [State; Huang, Xiaoli [State; Huang, Yanping [State; Han, Bo [State; Zhou, Qiang [State; Cui, Tian [State

    2017-07-19

    Tailoring the excitonic properties in two-dimensional monolayer transition metal dichalcogenides (TMDs) through strain engineering is an effective means to explore their potential applications in optoelectronics and nanoelectronics. Here we report pressure-tuned photon emission of trions and excitons in monolayer MoSe2 via a diamond anvil cell (DAC) through photoluminescence measurements and theoretical calculations. Under quasi-hydrostatic compressive strain, our results show neutral (X0) and charged (X–) exciton emission of monolayer MoSe2 can be effectively tuned by alcohol mixture vs inert argon pressure transmitting media (PTM). During this process, X– emission undergoes a continuous blue shift until reaching saturation, while X0 emission turns up splitting. The pressure-dependent charging effect observed in alcohol mixture PTM results in the increase of the X– exciton component and facilitates the pressure-tuned emission of X– excitons. This substantial tunability of X– and X0 excitons in MoSe2 can be extended to other 2D TMDs, which holds potential for developing strained and optical sensing devices.

  1. Quasiparticle and excitonic gaps of one-dimensional carbon chains.

    Science.gov (United States)

    Mostaani, E; Monserrat, B; Drummond, N D; Lambert, C J

    2016-06-01

    We report diffusion quantum Monte Carlo (DMC) calculations of the quasiparticle and excitonic gaps of hydrogen-terminated oligoynes and extended polyyne. The electronic gaps are found to be very sensitive to the atomic structure in these systems. We have therefore optimised the geometry of polyyne by directly minimising the DMC energy with respect to the lattice constant and the Peierls-induced carbon-carbon bond-length alternation. We find the bond-length alternation of polyyne to be 0.136(2) Å and the excitonic and quasiparticle gaps to be 3.30(7) and 3.4(1) eV, respectively. The DMC zone-centre longitudinal optical phonon frequency of polyyne is 2084(5) cm(-1), which is consistent with Raman spectroscopic measurements for large oligoynes.

  2. Multiple exciton generation in chiral carbon nanotubes: Density functional theory based computation

    Science.gov (United States)

    Kryjevski, Andrei; Mihaylov, Deyan; Kilina, Svetlana; Kilin, Dmitri

    2017-10-01

    We use a Boltzmann transport equation (BE) to study time evolution of a photo-excited state in a nanoparticle including phonon-mediated exciton relaxation and the multiple exciton generation (MEG) processes, such as exciton-to-biexciton multiplication and biexciton-to-exciton recombination. BE collision integrals are computed using Kadanoff-Baym-Keldysh many-body perturbation theory based on density functional theory simulations, including exciton effects. We compute internal quantum efficiency (QE), which is the number of excitons generated from an absorbed photon in the course of the relaxation. We apply this approach to chiral single-wall carbon nanotubes (SWCNTs), such as (6,2) and (6,5). We predict efficient MEG in the (6,2) and (6,5) SWCNTs within the solar spectrum range starting at the 2Eg energy threshold and with QE reaching ˜1.6 at about 3Eg, where Eg is the electronic gap.

  3. Band-Edge Exciton Fine Structure and Recombination Dynamics in InP/ZnS Colloidal Nanocrystals.

    Science.gov (United States)

    Biadala, Louis; Siebers, Benjamin; Beyazit, Yasin; Tessier, Mickaël D; Dupont, Dorian; Hens, Zeger; Yakovlev, Dmitri R; Bayer, Manfred

    2016-03-22

    We report on a temperature-, time-, and spectrally resolved study of the photoluminescence of type-I InP/ZnS colloidal nanocrystals with varying core size. By studying the exciton recombination dynamics we assess the exciton fine structure in these systems. In addition to the typical bright-dark doublet, the photoluminescence stems from an upper bright state in spite of its large energy splitting (∼100 meV). This striking observation results from dramatically lengthened thermalization processes among the fine structure levels and points to optical-phonon bottleneck effects in InP/ZnS nanocrystals. Furthermore, our data show that the radiative recombination of the dark exciton scales linearly with the bright-dark energy splitting for CdSe and InP nanocrystals. This finding strongly suggests a universal dangling bonds-assisted recombination of the dark exciton in colloidal nanostructures.

  4. Optical studies of high quality synthetic diamond

    International Nuclear Information System (INIS)

    Sharp, S.J.

    1999-01-01

    This thesis is concerned with the study of fundamental and defect induced optical properties of synthetic diamond grown using high pressure, high temperature (HPHT) synthesis or chemical vapour deposition (CVD). The primary technique used for investigation is cathodoluminescence (including imaging and decay-time measurements) in addition to other forms of optical spectroscopy. This thesis is timely in that the crystallinity and purity of synthetic diamond has increased ten fold over the last few years. The diamond exciton emission, which is easily quenched by the presence of defects, is studied in high quality samples in detail. In addition the ability now exists to engineer the isotopic content of synthetic diamond to a high degree of accuracy. The experimental chapters are divided as follows: Chapter 2: High resolution, low temperature spectra reveal a splitting of the free-exciton phonon recombination emission peaks and the bound-exciton zero phonon line. Included are measurements of the variation in intensity and decay-time as a function of temperature. Chapter 3: The shift in energy of the phonon-assisted free-exciton phonon replicas with isotopic content has been measured. The shift is in agreement with the results of interatomic force model for phonon scattering due to isotope disorder. Chapter 4: A study of the shift in energy with isotopic content of the diamond of the GR1 band due to the neutral vacancy has allowed a verification of the theoretical predictions due to the Jahn Teller effect. Chapter 5: The spatial distribution of the free-exciton luminescence is studied in HPHT synthetic and CVD diamond. A variation in intensity with distance from the surface is interpreted as a significant non-radiative loss of excitons to the surface. Chapter 6: The decay-times of all known self-interstitial related centres have been measured in order to calculate the concentration of these centres present in electron irradiated diamond. (author)

  5. Absorption Spectrum and Density of States of Square, Rectangular, and Triangular Frenkel Exciton Systems with Gaussian Diagonal Disorder

    Directory of Open Access Journals (Sweden)

    Ibrahim Avgin

    2017-01-01

    Full Text Available Using the coherent potential approximation, we investigate the effects of disorder on the optical absorption and the density of states of Frenkel exciton systems on square, rectangular, and triangular lattices with nearest-neighbor interactions and a Gaussian distribution of transition energies. The analysis is based on an elliptic integral approach that gives results over the entire spectrum. The results for the square lattice are in good agreement with the finite-array calculations of Schreiber and Toyozawa. Our findings suggest that the coherent potential approximation can be useful in interpreting the optical properties of two-dimensional systems with dominant nearest-neighbor interactions and Gaussian diagonal disorder provided the optically active states are Frenkel excitons.

  6. Spectral properties of excitons in the bilayer graphene

    Science.gov (United States)

    Apinyan, V.; Kopeć, T. K.

    2018-01-01

    In this paper, we consider the spectral properties of the bilayer graphene with the local excitonic pairing interaction between the electrons and holes. We consider the generalized Hubbard model, which includes both intralayer and interlayer Coulomb interaction parameters. The solution of the excitonic gap parameter is used to calculate the electronic band structure, single-particle spectral functions, the hybridization gap, and the excitonic coherence length in the bilayer graphene. We show that the local interlayer Coulomb interaction is responsible for the semimetal-semiconductor transition in the double layer system, and we calculate the hybridization gap in the band structure above the critical interaction value. The formation of the excitonic band gap is reported as the threshold process and the momentum distribution functions have been calculated numerically. We show that in the weak coupling limit the system is governed by the Bardeen-Cooper-Schrieffer (BCS)-like pairing state. Contrary, in the strong coupling limit the excitonic condensate states appear in the semiconducting phase, by forming the Dirac's pockets in the reciprocal space.

  7. Role of many-body effects in the coherent dynamics of excitons in low-temperature-grown GaAs

    Energy Technology Data Exchange (ETDEWEB)

    Webber, D.; Hacquebard, L.; Hall, K. C. [Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia B3H 4R2 (Canada); Liu, X.; Dobrowolska, M.; Furdyna, J. K. [Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556 (United States)

    2015-10-05

    Femtosecond four-wave mixing experiments on low-temperature-grown (LT-) GaAs indicate a polarization-dependent nonlinear optical response at the exciton, which we attribute to Coulomb-mediated coupling between excitons and electron-hole pairs simultaneously excited by the broad-bandwidth laser pulses. Strong suppression of the exciton response through screening by carriers injected by a third pump pulse was observed, an effect that is transient due to rapid carrier trapping. Our findings highlight the need to account for the complex interplay of disorder and many-body effects in the design of ultrafast optoelectronic devices using this material.

  8. Exciton emissions in alkali cyanides

    International Nuclear Information System (INIS)

    Weid, J.P. von der.

    1979-10-01

    The emissions of Alkali Cyanides X irradiated at low temperature were measured. In addition to the molecular (Frenkel Type) exciton emissions, another emitting centre was found and tentatively assigned to a charge transfer self trapped exciton. The nature of the molecular exciton emitting state is discussed. (Author) [pt

  9. Optically Controlled Quantum Dot Spins for Scaleable Quantum Computing

    National Research Council Canada - National Science Library

    Steel, Duncan G

    2005-01-01

    .... Our main achievements include working with a model system based on the exciton optical Bloch vector where we demonstrated the first solid state quantum logic device and made the first demonstration...

  10. Effective-mass model and magneto-optical properties in hybrid perovskites

    Science.gov (United States)

    Yu, Z. G.

    2016-06-01

    Hybrid inorganic-organic perovskites have proven to be a revolutionary material for low-cost photovoltaic applications. They also exhibit many other interesting properties, including giant Rashba splitting, large-radius Wannier excitons, and novel magneto-optical effects. Understanding these properties as well as the detailed mechanism of photovoltaics requires a reliable and accessible electronic structure, on which models of transport, excitonic, and magneto-optical properties can be efficiently developed. Here we construct an effective-mass model for the hybrid perovskites based on the group theory, experiment, and first-principles calculations. Using this model, we relate the Rashba splitting with the inversion-asymmetry parameter in the tetragonal perovskites, evaluate anisotropic g-factors for both conduction and valence bands, and elucidate the magnetic-field effect on photoluminescence and its dependence on the intensity of photoexcitation. The diamagnetic effect of exciton is calculated for an arbitrarily strong magnetic field. The pronounced excitonic peak emerged at intermediate magnetic fields in cyclotron resonance is assigned to the 3D±2 states, whose splitting can be used to estimate the difference in the effective masses of electron and hole.

  11. Comparison of additional boundary conditions based on thermoreflectance spectra of the Asub(n=1)-exciton in CdS crystals at oblique incidence

    International Nuclear Information System (INIS)

    Stoessel, W.; Wagner, H.J.

    1978-01-01

    Thermoreflectance spectra of the Asub(n=1)-exciton in CdS are measured at 8 K for angles of incidence of the light ranging from 5 0 to 85 0 , using three different spatial arrangements between the c-axis, the E- and k-vector of light. Additional boundary conditions of Pekar, Ting et al. Agarwal et al. are discussed for the first time in terms of optical constants. The refractive indices for these additional boundary conditions are derived, considering special features of CdS, such as optical anisotropy, exciton symmetry, and effective exciton mass anisotropy. Fitting calculations based on the experimental data show that Pekar's additional boundary condition gives the best agreement between theory and experiment. (author)

  12. The effect of excitons on CdTe solar cells

    International Nuclear Information System (INIS)

    Karazhanov, S. Zh.; Zhang, Y.; Mascarenhas, A.; Deb, S.

    2000-01-01

    Temperature and doping-level dependence of CdTe solar cells is investigated, taking into account the involvement of excitons on photocurrent transport. We show that the density of excitons in CdTe is comparable with that of minority carriers at doping levels ≥10 15 cm -3 . From the investigation of the dark-saturation current, we show that the product of electron and hole concentrations at equilibrium is several orders of magnitude more than the square of the intrinsic carrier concentration. With this assumption, we have studied the effect of excitons on CdTe solar cells, and the effect is negative. CdTe solar cell performance with excitons included agrees well with existing experimental results. (c) 2000 American Institute of Physics

  13. Exciton Seebeck effect in molecular systems

    Energy Technology Data Exchange (ETDEWEB)

    Yan, Yun-An, E-mail: yunan@nano.gznc.edu.cn [Guizhou Provincial Key Laboratory of Computational Nanomaterial Science, Guizhou Normal College, Guiyang, Guizhou 550018 (China); Cai, Shaohong [Guizhou Key Laboratory of Economic System Simulation, Guizhou University of Finance and Economics, Guiyang 550004 (China)

    2014-08-07

    We investigate the exciton dynamics under temperature difference with the hierarchical equations of motion. Through a nonperturbative simulation of the transient absorption of a heterogeneous trimer model, we show that the temperature difference causes exciton population redistribution and affects the exciton transfer time. It is found that one can reproduce not only the exciton population redistribution but also the change of the exciton transfer time induced by the temperature difference with a proper tuning of the site energies of the aggregate. In this sense, there exists a site energy shift equivalence for any temperature difference in a broad range. This phenomenon is similar to the Seebeck effect as well as spin Seebeck effect and can be named as exciton Seebeck effect.

  14. Temperature-dependent excitonic photoluminescence of hybrid organometal halide perovskite films

    KAUST Repository

    Wu, Kewei; Bera, Ashok; Ma, Chun; Du, Yuanmin; Yang, Yang; LI, LIANG; Wu, Tao

    2014-01-01

    Organometal halide perovskites have recently attracted tremendous attention due to their potential for photovoltaic applications, and they are also considered as promising materials in light emitting and lasing devices. In this work, we investigated in detail the cryogenic steady state photoluminescence properties of a prototypical hybrid perovskite CH3NH3PbI3-xClx. The evolution of the characteristics of two excitonic peaks coincides with the structural phase transition around 160 K. Our results further revealed an exciton binding energy of 62.3 ± 8.9 meV and an optical phonon energy of 25.3 ± 5.2 meV, along with an abnormal blue-shift of the band gap in the high-temperature tetragonal phase. This journal is

  15. Coherence properties of exciton-polariton OPO condensates in one and two dimensions

    DEFF Research Database (Denmark)

    Spano, R.; Cuadra, J.; Anton, C.

    2012-01-01

    We give an overview of the coherence properties of exciton-polariton condensates generated by optical parametric scattering. Different aspects of the first-order coherence (g((1))) have been investigated. The spatial coherence extension of a two-dimensional (2D) polariton system, below and at the...

  16. Entangled exciton states in quantum dot molecules

    Science.gov (United States)

    Bayer, Manfred

    2002-03-01

    Currently there is strong interest in quantum information processing(See, for example, The Physics of Quantum Information, eds. D. Bouwmeester, A. Ekert and A. Zeilinger (Springer, Berlin, 2000).) in a solid state environment. Many approaches mimic atomic physics concepts in which semiconductor quantum dots are implemented as artificial atoms. An essential building block of a quantum processor is a gate which entangles the states of two quantum bits. Recently a pair of vertically aligned quantum dots has been suggested as optically driven quantum gate(P. Hawrylak, S. Fafard, and Z. R. Wasilewski, Cond. Matter News 7, 16 (1999).)(M. Bayer, P. Hawrylak, K. Hinzer, S. Fafard, M. Korkusinski, Z.R. Wasilewski, O. Stern, and A. Forchel, Science 291, 451 (2001).): The quantum bits are individual carriers either on dot zero or dot one. The different dot indices play the same role as a "spin", therefore we call them "isospin". Quantum mechanical tunneling between the dots rotates the isospin and leads to superposition of these states. The quantum gate is built when two different particles, an electron and a hole, are created optically. The two particles form entangled isospin states. Here we present spectrocsopic studies of single self-assembled InAs/GaAs quantum dot molecules that support the feasibility of this proposal. The evolution of the excitonic recombination spectrum with varying separation between the dots allows us to demonstrate coherent tunneling of carriers across the separating barrier and the formation of entangled exciton states: Due to the coupling between the dots the exciton states show a splitting that increases with decreasing barrier width. For barrier widths below 5 nm it exceeds the thermal energy at room temperature. For a given barrier width, we find only small variations of the tunneling induced splitting demonstrating a good homogeneity within a molecule ensemble. The entanglement may be controlled by application of electromagnetic field. For

  17. Calculation of the Huang-Rhys parameter in spherical quantum dots: the optical deformation potential effect

    International Nuclear Information System (INIS)

    Hamma, M; Miranda, R P; Vasilevskiy, M I; Zorkani, I

    2007-01-01

    An accurate calculation of the exciton-phonon interaction matrix elements and Huang-Rhys parameter for nearly spherical nanocrystals (NCs) of polar semiconductor materials is presented. The theoretical approach is based on a continuum lattice dynamics model and the effective mass approximation for electronic states in the NCs. A strong confinement regime is considered for both excitons and optical phonons, taking into account both the Froehlich-type and optical deformation potential (ODP) mechanisms of the exciton-phonon interaction. The effects of exchange electron-hole interaction and possible hexagonal crystal structure of the underlying material are also taken into account. The theory is applied to CdSe and InP quantum dots. It is shown that the ODP mechanism, almost unimportant for CdSe, dominates the exciton-phonon coupling in small InP dots. The effect of the non-diagonal interaction, not included in the Huang-Rhys parameter, is briefly discussed

  18. The self-trapping of anion excitons in alkali halides at elastic deformation

    International Nuclear Information System (INIS)

    Tulepbergenov, S.K.; Dzhumanov, S.; Spivak-Lavrov, I.F.; Shunkeev, K.Sh.

    2001-01-01

    The self-trapping of electronic excitations (EE) (excitons, holes and electrons) in alkali halides (AH), fluorides and oxides plays an important roles in luminescence and defect formation. Therein the specific features of self-trapping of EE in various materials are essentially different. In particular, the self-trapping of excitons in some AH (i.e. alkali iodides and bromides) occurs with overcoming of the potential barrier and in other AH (e.g. alkali fluorides and chlorides) such a barrier is absent. Here we develop the continuum theory of self-trapping of within the adiabatic approximation elastically stressed AH. In the continuum model of solids the functional of the total energy of are interacting exciton-phonon system in the deformed ionic crystal just as in the undeformed crystal depends on the dilation Δ(r) described by the deformation potential of acoustic phonon, the electrostatic potential φ[r) due to the lattice polarization at optical lattice vibrations and the wave function of exciton chosen for hydro statically and uniaxially stressed 3D crystals. The functionals of the total energy of the interfacing exciton-phonon system E{Δ(r),φ(r),ψ(r)} are minimized relative to Δ, φ and ψ for the cases of isotropic and anisotropic 3D crystals. As a result, we obtained the functionals depending on μ and determined their possible extremum. We have show that the linear deformations under the hydrostatic and uniaxial stress at 80 K lead to the decreasing of the self trapping barrier for exciton and to the increasing of the luminescence of self-trapped excitons (STE). While the nonlinear deformations under the such stress at 80 K lead to the increasing of the self-trapping barrier for excitons and to the decreasing at the STE luminescence in AH. At T=0 K the small hydrostatic and uniaxial pressures lead to the same effects. Further at hydrostatic and uniaxial compressions of AH the minimums of the adiabatic potentials of quasifree and STE are shifted to

  19. Strongly bound excitons in monolayer PtS2 and PtSe2

    KAUST Repository

    Sajjad, M.

    2018-01-22

    Based on first-principles calculations, the structural, electronic, and optical properties of monolayers PtS2 and PtSe2 are investigated. The bond stiffnesses and elastic moduli are determined by means of the spring constants and strain-energy relations, respectively. Dynamic stability is confirmed by calculating the phonon spectra, which shows excellent agreement with experimental reports for the frequencies of the Raman-active modes. The Heyd-Scuseria-Ernzerhof functional results in electronic bandgaps of 2.66 eV for monolayer PtS2 and 1.74 eV for monolayer PtSe2. G0W0 calculations combined with the Bethe-Salpeter equation are used to predict the optical spectra and exciton binding energies (0.78 eV for monolayer PtS2 and 0.60 eV for monolayer PtSe2). It turns out that the excitons are strongly bound and therefore very stable against external perturbations.

  20. Optical Studies of Excitonic Effects at Two-Dimensional Nanostructure Interfaces

    Science.gov (United States)

    Ajayi, Obafunso Ademilolu

    Atomically thin two-dimensional nanomaterials such as graphene and transition metal dichalcogenides (TMDCs) have seen a rapid growth of exploration since the isolation of monolayer graphene. These materials provide a rich field of study for physics and optoelectronics applications. Many applications seek to combine a two dimensional (2D) material with another nanomaterial, either another two dimensional material or a zero (0D) or one dimensional (1D) material. The work in this thesis explores the consequences of these interactions from 0D to 2D. We begin in Chapter 2 with a study of energy transfer at 0D-2D interfaces with quantum dots and graphene. In our work we seek to maximize the rate of energy transfer by reducing the distance between the materials. We observe an interplay with the distance-dependence and surface effects from our halogen terminated quantum dots that affect our observed energy transfer. In Chapter 3 we study supercapacitance in composite graphene oxide-carbon nanotube electrodes. At this 2D-1D interface we observe a compounding effect between graphene oxide and carbon nanotubes. Carbon nanotubes increase the accessible surface area of the supercapacitors and improve conductivity by forming a conductive pathway through electrodes. In Chapter 4 we investigate effective means of improving sample quality in TMDCs and discover the importance of the monolayer interface. We observe a drastic improvement in photoluminescence when encapsulating our TMDCs with Boron Nitride. We measure spectral linewidths approaching the intrinsic limit due to this 2D-2D interface. We also effectively reduce excess charge and thus the trion-exciton ratio in our samples through substrate surface passivation. In Chapter 5 we briefly discuss our investigations on chemical doping, heterostructures and interlayer decoupling in ReS2. We observe an increase in intensity for p-doped MoS2 samples. We investigated the charge transfer exciton previously identified in

  1. Self-reflection in a system of excitons and biexcitons in semiconductors

    International Nuclear Information System (INIS)

    Khadzhi, P I; Lyakhomskaya, K D

    1999-01-01

    The characteristic features of the self-reflection of a powerful electromagnetic wave in a system of coherent excitons and biexcitons in semiconductors were investigated as one of the manifestations of the nonlinear optical skin effect. It was found that a monotonically decreasing standing wave with an exponentially falling spatial tail is formed in the surface region of a semiconductor. Under the influence of the field of a powerful pulse, an optically homogeneous medium is converted into one with distributed feedback. The appearance of spatially separated narrow peaks of the refractive index, extinction coefficient, and reflection coefficient is predicted. (nonlinear optical phenomena)

  2. Effect of disorder on exciton dissociation in conjugated polymers

    International Nuclear Information System (INIS)

    Feng Yuwen; Zhao Hui; Chen Yuguang; Yan Yonghong

    2017-01-01

    By using a multi-configurational time-dependent Hartree–Fock (MCTDHF) method for the time-dependent Schrödinger equation and a Newtonian equation of motion for lattice, we investigate the disorder effects on the dissociation process of excitons in conjugated polymer chains. The simulations are performed within the framework of an extended version of the Su–Schrieffer–Heeger model modified to include on-site disorder, off-diagonal, electron–electron interaction, and an external electric field. Our results show that Coulomb correlation effects play an important role in determining the exciton dissociation process. The electric field required to dissociate an exciton can practically impossibly occur in a pure polymer chain, especially in the case of triplet exciton. However, when the on-site disorder effects are taken into account, this leads to a reduction in mean dissociation electric fields. As the disorder strength increases, the dissociation field decreases effectively. On the contrary, the effects of off-diagonal disorder are negative in most cases. Moreover, the dependence of exciton dissociation on the conjugated length is also discussed. (paper)

  3. Triplet exciton dynamics

    International Nuclear Information System (INIS)

    Strien, A.J. van.

    1981-01-01

    Results are presented of electron spin echo experiments combined with laser flash excitation on triplet states of aromatic molecules. Some of the theoretical and experimental aspects of the photoexcited triplet state are discussed in detail and the electron spin echo spectrometers and laser systems are described. All the experiments described in this thesis were performed at liquid helium temperatures. An account is given of the ESE experiments performed on the photoexcited, non-radiative, triplet state of pentacene in napthalene. This is an example of the ESE technique being used to ascertain the zero-field splitting parameters, the populating and depopulating rates, and the orientation of the pentacene molecules in the naphthalene host. A combination of high resolution laser flash excitation and electron-spin echoes in zero-magnetic field allowed the author to observe directly k(vector)→k(vector)' exciton scattering processes in the one-dimensional triplet excitons in tetrachlorobenzene for the first time. Additional experimental data about exciton scattering is provided and a study of the orientational dependence of the spin-lattice relaxation of the triplet excitons in an external magnetic field is described. (Auth.)

  4. Plasmon-exciton-polariton lasing

    NARCIS (Netherlands)

    Ramezani, M.; Halpin, A.; Fernández-Dominguez, A.I.; Feist, J.; Rodriguez, S.R.K.; Gómez-Rivas, J.; Garcia-Vidal, F.J.

    2016-01-01

    Strong coupling of Frenkel excitons with surface plasmons leads to the formation of bosonic quasi-particles known as plasmon-exciton-polaritons (PEPs).Localized surface plasmons in nanoparticles are lossy due to radiative and nonradiative decays, which has hampered the realization of polariton

  5. Composition-Dependent Energy Splitting between Bright and Dark Excitons in Lead Halide Perovskite Nanocrystals.

    Science.gov (United States)

    Chen, Lan; Li, Bin; Zhang, Chunfeng; Huang, Xinyu; Wang, Xiaoyong; Xiao, Min

    2018-03-14

    Perovskite semiconductor nanocrystals with different compositions have shown promise for applications in light-emitting devices. Dark excitonic states may suppress light emission from such nanocrystals by providing an additional nonradiative recombination channel. Here, we study the composition dependence of dark exciton dynamics in nanocrystals of lead halides by time-resolved photoluminescence spectroscopy at cryogenic temperatures. The presence of a spin-related dark state is revealed by magneto-optical spectroscopy. The energy splitting between bright and dark states is found to be highly sensitive to both halide elements and organic cations, which is explained by considering the effects of size confinement and charge screening, respectively, on the exchange interaction. These findings suggest the possibility of manipulating dark exciton dynamics in perovskite semiconductor nanocrystals by composition engineering, which will be instrumental in the design of highly efficient light-emitting devices.

  6. Structural and optical studies of local disorder sensitivity in natural organic-inorganic self-assembled semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Vijaya Prakash, G; Pradeesh, K [Nanophotonics Lab, Department of Physics, Indian Institute of Technology Delhi, New Delhi (India); Ratnani, R; Saraswat, K [Department of Pure and Applied Chemistry, MDS University, Ajmer (India); Light, M E [School of Chemistry, University of Southampton, Southampton (United Kingdom); Baumberg, J J, E-mail: prakash@physics.iitd.ac.i [Nanophotonic Centre, Cavendish Laboratory, University Cambridge, Cambridge CB3 OHE (United Kingdom)

    2009-09-21

    The structural and optical spectra of two related lead iodide (PbI) based self-assembled hybrid organic-inorganic semiconductors are compared. During the synthesis, depending on the bridging of organic moiety intercalated between the PbI two-dimensional planes, different crystal structures are produced. These entirely different networks show different structural and optical features, including excitonic bandgaps. In particular, the modified organic environment of the excitons is sensitive to the local disorder both in single crystal and thin film forms. Such information is vital for incorporating these semiconductors into photonic device architectures.

  7. Quenching of exciton luminescence due to impact ionization and mechanisms of electron relaxation in cadmium sulphide

    International Nuclear Information System (INIS)

    Kagan, V.D.; Karpenko, S.L.; Katilyus, R.

    1989-01-01

    Quenching of exciton luminescence in the constant electric field in cadmium sulfide at 1.8K, caused by impact ionization of free and delocalization of bound excitons by hot electrons is observed. When the field is increase up to 1 kW/cm continuous transfer from the Taundsen-Shockley law to the Davydov-Wolf one takes place. Among the samples studied pure samples are distinguished by the exciton spectrum, where, as it is shown in the work, the high-energy electrons lose quasipulse, radiating spontaneously piezophonons; in other samples scattering on impurities prevails. Theoretical processing of data on the bound exciton radiation line quenching in the moderate field region presents about 10 -4 values in pure and about 5x10 -6 cm ones in other samples for the 4 MeV energy electron free flight length. So, the optical methods used allowed one to determine high-energy electron relaxation mechanisms, prevailing in CdS at low temperature

  8. Phase Diagram of the Bose Condensation of Interwell Excitons in GaAs/AlGaAs Double Quantum Wells

    DEFF Research Database (Denmark)

    Dremin, A. A.; Timofeev, V. B.; Larionov, A. V.

    2002-01-01

    The luminescence of interwell excitons in GaAs/AlGaAs double quantum wells (n–i–n heterostructures) with large-scale fluctuations of random potential in the heteroboundary planes was studied at low temperatures down to 0.5 K. The properties of excitons whose photoexcited electron and hole...... was coated with a metal mask containing special openings (windows) of a micron size or smaller. Both photoexcitation and observation of luminescence were performed through these windows by the fiber optic technique. At low pumping powers, the interwell excitons were strongly localized because of the residual...... charged impurities, and the corresponding photoluminescence line was nonuniformly broadened. As the laser excitation power increased, a narrow line due to delocalized excitons arose in a threshold-like manner, after which its intensity rapidly increased with growing pumping and the line itself narrowed...

  9. Excitons in the rare gas solids

    International Nuclear Information System (INIS)

    1988-01-01

    Excitons play a prominent role in the chemistry and physics of condensed matter. Excitons in the rare gas solids, the prototypical van der Waals insulators, will be the focus of the remainder of this report. The goal here is to investigate the controversies surrounding the description of excitons in insulators and, therefore the simplest class of these solids, namely the rare gas solids, is chosen as the exemplary system. Specific problems associated with molecular crystals are, therefore, avoided and only the salient features of excitons are thus considered. 47 refs., 9 figs., 4 tabs

  10. Plasmon-exciton polaritons in two-dimensional semiconductor/metal interfaces

    Science.gov (United States)

    Gonçalves, P. A. D.; Bertelsen, L. P.; Xiao, Sanshui; Mortensen, N. Asger

    2018-01-01

    The realization and control of polaritons is of paramount importance in the prospect of novel photonic devices. Here, we investigate the emergence of plasmon-exciton polaritons in hybrid structures consisting of a two-dimensional transition-metal dichalcogenide (TMDC) deposited onto a metal substrate or coating a metallic thin film. We determine the polaritonic spectrum and show that, in the former case, the addition of a top dielectric layer and, in the latter case, the thickness of the metal film can be used to tune and promote plasmon-exciton interactions well within the strong-coupling regime. Our results demonstrate that Rabi splittings exceeding 100 meV can readily be achieved in planar dielectric/TMDC/metal structures under ambient conditions. We thus believe that this Rapid Communication provides a simple and intuitive picture to tailor strong coupling in plexcitonics with potential applications for engineering compact photonic devices with tunable optical properties.

  11. Controlling the exciton emission of gold coated GaAs-AlGaAs core-shell nanowires with an organic spacer layer

    Science.gov (United States)

    Kaveh, M.; Gao, Q.; Jagadish, C.; Ge, J.; Duscher, G.; Wagner, H. P.

    2016-12-01

    Excitons are the most prominent optical excitations and controlling their emission is an important step towards new optical devices. We have investigated the exciton emission from uncoated and gold/aluminum quinoline (Alq3) coated GaAs-AlGaAs-GaAs core-shell nanowires (NWs) using temperature-, intensity- and polarization dependent photoluminescence (PL). Plasmonic GaAs-AlGaAs-GaAs NWs with a ˜10 nm thick Au coating but without an Alq3 spacer layer reveal a significant reduction of the PL intensity of the exciton emission compared with the uncoated NW sample. Plasmonic NW samples with the same nominal Au coverage and an additional Alq3 interlayer of 3 or 6 nm thickness show a clearly stronger PL intensity which increases with rising Alq3 spacer thickness. Time-resolved (TR) PL measurements reveal an increase of the exciton decay rate by a factor of up to two with decreasing Alq3 spacer thickness suggesting the presence of Förster energy transfer from NW excitons to plasmon oscillations in the gold film. The weak change of the decay time, however, indicates that Förster energy-transfer is only partially responsible for the PL quenching in the gold coated NWs. The main reason for the reduction of the PL emission is attributed to a gold induced band-bending in the GaAs NW core which causes exciton dissociation. With increasing Alq3 spacer thickness the band-bending decreases leading to a reduction of the exciton dissociation and PL quenching. Our interpretation is supported by electron energy loss spectroscopy measurements which show a signal reduction and blue shift of defect (possibly EL2) transitions when gold particles are deposited on NWs compared with bare or Alq3 coated NWs.

  12. A toy model to investigate the existence of excitons in the ground state of strongly-correlated semiconductor

    Science.gov (United States)

    Karima, H. R.; Majidi, M. A.

    2018-04-01

    Excitons, quasiparticles associated with bound states between an electron and a hole and are typically created when photons with a suitable energy are absorbed in a solid-state material. We propose to study a possible emergence of excitons, created not by photon absorption but the effect of strong electronic correlations. This study is motivated by a recent experimental study of a substrate material SrTiO3 (STO) that reveals strong exitonic signals in its optical conductivity. Here we conjecture that some excitons may already exist in the ground state as a result of the electronic correlations before the additional excitons being created later by photon absorption. To investigate the existence of excitons in the ground state, we propose to study a simple 4-energy-level model that mimics a situation in strongly-correlated semiconductors. The four levels are divided into two groups, lower and upper groups separated by an energy gap, Eg , mimicking the valence and the conduction bands, respectively. Further, we incorporate repulsive Coulomb interactions between the electrons. The model is then solved by exact diagonalization method. Our result shows that the toy model can demonstrate band gap widening or narrowing and the existence of exciton in the ground state depending on interaction parameter values.

  13. Excitons

    Energy Technology Data Exchange (ETDEWEB)

    Kozhushner, M

    1975-06-01

    The theory of quasi particles is explained to layman readers and the significance of the discovery of excitons is pointed out. New possibilities of the study of electron-hole interactions and of superconductivity are indicated.

  14. Optical density of states in ultradilute GaAsN alloy: Coexistence of free excitons and impurity band of localized and delocalized states

    Energy Technology Data Exchange (ETDEWEB)

    Bhuyan, Sumi; Pal, Bipul; Bansal, Bhavtosh, E-mail: bhavtosh@iiserkol.ac.in [Indian Institute of Science Education and Research Kolkata, Mohanpur Campus, Nadia 741252, West Bengal (India); Das, Sanat K.; Dhar, Sunanda [Department of Electronic Science, University of Calcutta, 92 A.P.C. Road, Kolkata 700009 (India)

    2014-07-14

    Optically active states in liquid phase epitaxy-grown ultra-dilute GaAsN are studied. The feature-rich low temperature photoluminescence spectrum has contributions from excitonic band states of the GaAsN alloy, and two types of defect states—localized and extended. The degree of delocalization for extended states both within the conduction and defect bands, characterized by the electron temperature, is found to be similar. The degree of localization in the defect band is analyzed by the strength of the phonon replicas. Stronger emission from these localized states is attributed to their giant oscillator strength.

  15. Synthesis of zinc oxide microrods and nano-fibers with dominant exciton emission at room temperature

    Energy Technology Data Exchange (ETDEWEB)

    Ramos-Brito, F., E-mail: fro_brito@yahoo.com.m [Laboratorio de Materiales Optoelectronicos del Centro de Ciencias de Sinaloa, Ave. de las Americas 2771 Col. Villa Universidad 80010, Culiacan, Sinaloa (Mexico); Alejo-Armenta, C. [Laboratorio de Materiales Optoelectronicos del Centro de Ciencias de Sinaloa, Ave. de las Americas 2771 Col. Villa Universidad 80010, Culiacan, Sinaloa (Mexico); Garcia-Hipolito, M. [Departamento de Materiales Metalicos y Ceramicos, Instituto de Investigaciones en Materiales, Universidad Nacional Autonoma de Mexico, AP 70-360, Coyoacan 04510, DF (Mexico); Camarillo, E.; Hernandez A, J. [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, AP 20-364, Alvaro Obregon 01000, DF (Mexico); Falcony, C. [Departamento de Fisica, CINVESTAV-IPN, AP 14-740, 07000, DF (Mexico); Murrieta S, H. [Instituto de Fisica, Universidad Nacional Autonoma de Mexico, AP 20-364, Alvaro Obregon 01000, DF (Mexico)

    2011-05-15

    Employing a simple chemical synthesis method, hexagonal-shaped zinc oxide microrods and zinc oxide nano-fibers were deposited on pyrex-glass and aluminum substrates, respectively. Both kinds of deposits showed zincite crystalline phase with lattice parameters: a=3.2498 A and c=5.2066 A. Microrods showed very uniform wide and large sizes of around 1 and 10 {mu}m, respectively. Both deposits were homogeneous over all substrate surfaces. Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0]and [0 0 0 1]directions. The principal optical characteristics for both microrods and nano-fibers were: a) room-temperature photo and cathodo-luminescent spectra with strong exciton emission centered around 390 nm and with FWHMs around 125 and 160 meV, respectively, b) poor photo and cathode-luminescent emissions in the visible region of the electromagnetic spectrum, c) energy band gap of 3.32 eV, d) good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission and e) good ZnO stoichiometry endorsed by photoluminescent results. These characteristics make of these microrods and nano-fibers good for potential photonic applications. - Research highlights: {yields} Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0]and [0 0 0 1]directions. {yields} Microrods and nano-fibers resulted with good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission. {yields} The wet chemical method is appropriated for deposition of microrods and nano-fibers with the desired optical properties for its possible application in photonics.

  16. Synthesis of zinc oxide microrods and nano-fibers with dominant exciton emission at room temperature

    International Nuclear Information System (INIS)

    Ramos-Brito, F.; Alejo-Armenta, C.; Garcia-Hipolito, M.; Camarillo, E.; Hernandez A, J.; Falcony, C.; Murrieta S, H.

    2011-01-01

    Employing a simple chemical synthesis method, hexagonal-shaped zinc oxide microrods and zinc oxide nano-fibers were deposited on pyrex-glass and aluminum substrates, respectively. Both kinds of deposits showed zincite crystalline phase with lattice parameters: a=3.2498 A and c=5.2066 A. Microrods showed very uniform wide and large sizes of around 1 and 10 μm, respectively. Both deposits were homogeneous over all substrate surfaces. Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0] and [0 0 0 1] directions. The principal optical characteristics for both microrods and nano-fibers were: a) room-temperature photo and cathodo-luminescent spectra with strong exciton emission centered around 390 nm and with FWHMs around 125 and 160 meV, respectively, b) poor photo and cathode-luminescent emissions in the visible region of the electromagnetic spectrum, c) energy band gap of 3.32 eV, d) good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission and e) good ZnO stoichiometry endorsed by photoluminescent results. These characteristics make of these microrods and nano-fibers good for potential photonic applications. - Research highlights: → Microrods and nano-fibers resulted with good optical quality and with preferential crystalline growth in [1 0 1 0] and [0 0 0 1] directions. → Microrods and nano-fibers resulted with good emission efficiency supported by the not-required high energy densities to obtain strong exciton emission. → The wet chemical method is appropriated for deposition of microrods and nano-fibers with the desired optical properties for its possible application in photonics.

  17. Excitons

    International Nuclear Information System (INIS)

    Kozhushner, M.

    1975-01-01

    The theory of quasi particles is explained to layman readers and the significance of the discovery of excitons is pointed out. New possibilities of the study of electron-hole interactions and of superconductivity are indicated. (L.O.)

  18. Interaction and dephasing of center-of-mass quantized excitons in wide ZnSe/Zn0.94Mg0.06Se quantum wells

    DEFF Research Database (Denmark)

    Wagner, Hans Peter; Schätz, A.; Maier, R.

    1998-01-01

    We investigate the interaction and dephasing of the excitons in wide ZnSe/Zn0.94Mg0.06Se quantum wells by spectrally resolved, femtosecond four-wave mixing (FWM). Polarization-dependent measurements indicate that excitation-induced dephasing is the dominant FWM process. The biexcitons of the center...... repulsion for coherent excitons. The exciton interaction rates with acoustic and optical phonons are deduced by their temperature dependencies. The acoustic-phonon scattering is found to be strongly reduced in the investigated wide wells due to the reduced accessible phonon wave vector....

  19. Exciton dynamics in GaAs/AlxGa1-xAs quantum wells

    DEFF Research Database (Denmark)

    Litvinenko, K.; Birkedal, Dan; Lyssenko, V. G.

    1999-01-01

    The changes induced in the optical absorption spectrum of a GaAs/AlxGa1-xAs multiple quantum well due to a photoexcited carrier distribution are reexamined. We use a femtosecond pump-probe technique to excite excitons and free electron-hole pairs. We find that for densities up to 10(11) cm(-2...

  20. First-principles calculation of optical absorption spectra in conjugated polymers: Role of electron-hole interaction

    International Nuclear Information System (INIS)

    Rohlfing, Michael; Tiago, M.L.; Louie, Steven G.

    2000-01-01

    Experimental and theoretical studies have shown that excitonic effects play an important role in the optical properties of conjugated polymers. The optical absorption spectrum of trans-polyacetylene, for example, can be understood as completely dominated by the formation of exciton bound states. We review a recently developed first-principles method for computing the excitonic effects and optical spectrum, with no adjustable parameters. This theory is used to study the absorption spectrum of two conjugated polymers: trans-polyacetylene and poly-phenylene-vinylene(PPV)

  1. First-principles calculation of optical absorption spectra in conjugated polymers: Role of electron-hole interaction

    Energy Technology Data Exchange (ETDEWEB)

    Rohlfing, Michael; Tiago, M.L.; Louie, Steven G.

    2000-03-20

    Experimental and theoretical studies have shown that excitonic effects play an important role in the optical properties of conjugated polymers. The optical absorption spectrum of trans-polyacetylene, for example, can be understood as completely dominated by the formation of exciton bound states. We review a recently developed first-principles method for computing the excitonic effects and optical spectrum, with no adjustable parameters. This theory is used to study the absorption spectrum of two conjugated polymers: trans-polyacetylene and poly-phenylene-vinylene(PPV).

  2. Phonon-assisted exciton formation in ZnO/(Zn, Mg)O single quantum wells grown on C-plane oriented substrates

    International Nuclear Information System (INIS)

    Béaur, L.; Bretagnon, T.; Guillet, T.; Brimont, C.; Gallart, M.; Gil, B.; Gilliot, P.; Morhain, C.

    2013-01-01

    We report on absorption phenomena in ZnO/(Zn, Mg)O quantum wells grown along the c-axis by molecular beam epitaxy. The optical properties of such quantum wells are affected by a huge internal electric field. For wide quantum wells the absorption is driven by Quantum Confined Stark Effect. Phonon-assisted formation of excitons is observed in the case of thin quantum wells. The physical origin of these hot excitons is determined by using both low temperature (T=10 K) photoluminescence excitation spectroscopy and reflectivity measurements. -- Highlights: ► High structural quality ZnO/(Zn, Mg)O quantum wells are growth along the polar c-direction. ► Indirect phonon-assisted formation of excitons in the thin single quantum wells. ► Strong internal electric field present in polar heterostructures prevents the observation of hot excitons

  3. Resonant exciton-phonon coupling in ZnO nanorods at room temperature

    Directory of Open Access Journals (Sweden)

    Soumee Chakraborty

    2011-09-01

    Full Text Available Vibronic and optoelectronic properties, along with detailed studies of exciton-phonon coupling at room temperature (RT for random and aligned ZnO nanorods are reported. Excitation energy dependent Raman studies are performed for detailed analysis of multi-phonon processes in the nanorods. We report here the origin of coupling between free exciton and its associated phonon replicas, including its higher order modes, in the photoluminescence spectra at RT. Resonance of excitonic electron and resonating first order zone center LO phonon, invoked strongly by Frolich interaction, are made responsible for the observed phenomenon.

  4. Optical response of confined excitons in GaInAsSb/GaSb Quantum Dots heterostructures

    Energy Technology Data Exchange (ETDEWEB)

    Sanchez-Cano, R [Departamento de Fisica, Universidad Autonoma de Occidente, A.A. 2790, Cali (Colombia); Tirado-Mejia, L; Fonthal, G; Ariza-Calderon, H [Laboratorio de Optoelectronica, Universidad del Quindio, A.A. 4603 Armenia (Colombia); Porras-Montenegro, N, E-mail: rsanchez40@gmail.co [Departamento de Fisica, Universidad del Valle, A.A. 25360, Cali (Colombia)

    2009-05-01

    The narrow-gap Ga{sub 1-x}In{sub x}As{sub y}Sb{sub 1-y} compounds are suitable materials for heterostructure devices operating in the infrared wavelength range. In these compounds grown by liquid phase epitaxy over GaSb single crystals, for x and y values in the range of 0.10 to 0.14 for both variables, the photoluminescence optical response at 12K is blue-shifted by 20 meV related to the photoreflectance response. We believe this behavior is due to possible higher electronic confinement in some places of the heterostructure, possibly formed in the interface during the growth process. In order to explain this behavior, in this work we study the exciton recombination energy in spherical Quantum Dots (QDs) on Ga{sub 1-x}In{sub x}As{sub y}Sb{sub 1-y}/GaSb, using the variational procedure within the effective-mass approximation and considering an electron in a Type I band alignment formed by two semiconductors with similar parabolic conduction bands. Our results are in good agreement with recent experimental results.

  5. Effect of the depolarization field on coherent optical properties in semiconductor quantum dots

    Science.gov (United States)

    Mitsumori, Yasuyoshi; Watanabe, Shunta; Asakura, Kenta; Seki, Keisuke; Edamatsu, Keiichi; Akahane, Kouichi; Yamamoto, Naokatsu

    2018-06-01

    We study the photon echo spectrum of self-assembled semiconductor quantum dots using femtosecond light pulses. The spectrum shape changes from a single-peaked to a double-peaked structure as the time delay between the two excitation pulses is increased. The spectrum change is reproduced by numerical calculations, which include the depolarization field induced by the biexciton-exciton transition as well as the conventional local-field effect for the exciton-ground-state transition in a quantum dot. Our findings suggest that various optical transitions in tightly localized systems generate a depolarization field, which renormalizes the resonant frequency with a change in the polarization itself, leading to unique optical properties.

  6. Type II InAs/GaAsSb quantum dots: Highly tunable exciton geometry and topology

    Energy Technology Data Exchange (ETDEWEB)

    Llorens, J. M.; Wewior, L.; Cardozo de Oliveira, E. R.; Alén, B., E-mail: benito.alen@csic.es [IMM-Instituto de Microelectrónica de Madrid (CNM-CSIC), Isaac Newton 8, PTM, E-28760 Tres Cantos, Madrid (Spain); Ulloa, J. M.; Utrilla, A. D.; Guzmán, A.; Hierro, A. [Institute for Systems based on Optoelectronics and Microtechnology (ISOM), Universidad Politécnica de Madrid, Ciudad Universitaria s/n, 28040 Madrid (Spain)

    2015-11-02

    External control over the electron and hole wavefunctions geometry and topology is investigated in a p-i-n diode embedding a dot-in-a-well InAs/GaAsSb quantum structure with type II band alignment. We find highly tunable exciton dipole moments and largely decoupled exciton recombination and ionization dynamics. We also predicted a bias regime where the hole wavefunction topology changes continuously from quantum dot-like to quantum ring-like as a function of the external bias. All these properties have great potential in advanced electro-optical applications and in the investigation of fundamental spin-orbit phenomena.

  7. Inelastic scattering of neutrons by laser photons and excitons in crystals

    International Nuclear Information System (INIS)

    Agranovich, V.M.; Lalov, I.J.

    1975-01-01

    The cross section for the neutron scattering by photons sharply increases in crystals. In view of the fact that a propagating photon in a crystal (polariton), being the superposition of transverse photons and Coulomb excitations (optical phonons, excitons, etc.), involves in the motion also a nucleus subsystem, the cross section for the neutron scattering on the photon turns out to be proportional to the cross section for neutron scattering on nuclei and to the strength function of phonons at the polariton frequency. Numerical estimates for the cross section of the noncoherent photon absorption by a neutron in the case of a LiH crystal in the presence of an intense, electromagnetic radiation point to the possibility of an action of neutron fluxes by laser radiation. A similar effect of involvement (superposition) also takes place for excitons. This fact can be used for calculations of the cross section for neutron inelastic scattering by excitons, which is proportional to the scattering of neutron on nuclei cross section. The paper also discussed the effect of laser radiation of neutron-induced nuclear reaction (radiative capture and threshold reactions)

  8. Models of coherent exciton condensation

    International Nuclear Information System (INIS)

    Littlewood, P B; Eastham, P R; Keeling, J M J; Marchetti, F M; Simons, B D; Szymanska, M H

    2004-01-01

    That excitons in solids might condense into a phase-coherent ground state was proposed about 40 years ago, and has been attracting experimental and theoretical attention ever since. Although experimental confirmation has been hard to come by, the concepts released by this phenomenon have been widely influential. This tutorial review discusses general aspects of the theory of exciton and polariton condensates, focusing on the reasons for coherence in the ground state wavefunction, the BCS to Bose crossover(s) for excitons and for polaritons, and the relationship of the coherent condensates to standard lasers

  9. Models of coherent exciton condensation

    Energy Technology Data Exchange (ETDEWEB)

    Littlewood, P B [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Eastham, P R [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Keeling, J M J [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Marchetti, F M [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Simons, B D [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom); Szymanska, M H [Theory of Condensed Matter, Cavendish Laboratory, Cambridge CB3 0HE (United Kingdom)

    2004-09-08

    That excitons in solids might condense into a phase-coherent ground state was proposed about 40 years ago, and has been attracting experimental and theoretical attention ever since. Although experimental confirmation has been hard to come by, the concepts released by this phenomenon have been widely influential. This tutorial review discusses general aspects of the theory of exciton and polariton condensates, focusing on the reasons for coherence in the ground state wavefunction, the BCS to Bose crossover(s) for excitons and for polaritons, and the relationship of the coherent condensates to standard lasers.

  10. Density-dependent squeezing of excitons in highly excited semiconductors

    International Nuclear Information System (INIS)

    Nguyen Hong Quang.

    1995-07-01

    The time evolution from coherent states to squeezed states of high density excitons is studied theoretically based on the boson formalism and within the Random Phase Approximation. Both the mutual interaction between excitons and the anharmonic exciton-photon interaction due to phase-space filling of excitons are taken into account. It is shown that the exciton squeezing depends strongly on the exciton density in semiconductors and becomes smaller with increasing the latter. (author). 16 refs, 2 figs

  11. Excitonic recombination dynamics in non-polar GaN/AlGaN quantum wells

    Science.gov (United States)

    Rosales, D.; Gil, B.; Bretagnon, T.; Guizal, B.; Zhang, F.; Okur, S.; Monavarian, M.; Izyumskaya, N.; Avrutin, V.; Özgür, Ü.; Morkoç, H.; Leach, J. H.

    2014-02-01

    The optical properties of GaN/Al0.15Ga0.85N multiple quantum wells are examined in 8 K-300 K temperature range. Both polarized CW and time resolved temperature-dependent photoluminescence experiment are performed so that we can deduce the relative contributions of the non-radiative and radiative recombination processes. From the calculation of the proportion of the excitonic population having wave vector in the light cone, we can deduce the variation of the radiative decay time with temperature. We find part of the excitonic population to be localized in concert with the report of Corfdir et al. (Jpn. J. Appl. Phys., Part 2 52, 08JC01 (2013)) in case of a-plane quantum wells.

  12. Photoluminescence and Confinement of Excitons in Disordered Porous Films

    Energy Technology Data Exchange (ETDEWEB)

    Bondar, N. V., E-mail: jbond@iop.kiev.ua; Brodin, M. S. [National Academy of Sciences of Ukraine, Institute of Physics (Ukraine); Brodin, A. M. [National Technical University of Ukraine “KPI” (Ukraine); Matveevskaya, N. A. [National Academy of Sciences of Ukraine, Institute for Single Crystals (Ukraine)

    2016-03-15

    The exciton confinement effect in quantum dots at the surface of SiO{sub 2} spheres and the percolation phase transition in films based on a mixture of pure SiO{sub 2} spheres and spheres covered by CdS quantum dots (SiO{sub 2}/CdS nanoparticles) are studied. It is found that, due to the high surface energy of spheres, the quantum dots deposited onto their surface are distorted, which modifies the exciton confinement effect: the effect is retained only in one direction, the direction normal to the surface of the spheres. As a result, the energy of the exciton ground state exhibits a complex dependence on both the quantum-dot radius and sphere size. In the optical spectra of films based on this mixture, the clustering of small-sized nanoparticles and then, at a critical concentration of nanoparticles of ~60%, the formation of a percolation cluster are detected for the first time. The critical concentration is twice higher than the corresponding quantity given by the model of geometrical “colored percolation”, which is a consequence of interaction between submicrometer nanoparticles. The relation between the basic parameters of the percolation transition, such as the film porosity, coordination number, and the quantity defining the number of particles in the percolation cluster, is obtained and analyzed.

  13. PbSe Nanocrystal Excitonic Solar Cells

    KAUST Repository

    Choi, Joshua J.

    2009-11-11

    We report the design, fabrication, and characterization of colloidal PbSe nanocrystal (NC)-based photovoltaic test structures that exhibit an excitonic solar cell mechanism. Charge extraction from the NC active layer is driven by a photoinduced chemical potential energy gradient at the nanostructured heterojunction. By minimizing perturbation to PbSe NC energy levels and thereby gaining insight into the "intrinsic" photovoltaic properties and charge transfer mechanism of PbSe NC, we show a direct correlation between interfacial energy level offsets and photovoltaic device performance. Size dependent PbSe NC energy levels were determined by cyclic voltammetry and optical spectroscopy and correlated to photovoltaic measurements. Photovoltaic test structures were fabricated from PbSe NC films sandwiched between layers of ZnO nanoparticles and PEDOT:PSS as electron and hole transporting elements, respectively. The device current-voltage characteristics suggest a charge separation mechanism that Is distinct from previously reported Schottky devices and consistent with signatures of excitonic solar cells. Remarkably, despite the limitation of planar junction structure, and without film thickness optimization, the best performing device shows a 1-sun power conversion efficiency of 3.4%, ranking among the highest performing NC-based solar cells reported to date. © 2009 American Chemical Society.

  14. Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged, and free excitons

    Science.gov (United States)

    Tongay, Sefaattin; Suh, Joonki; Ataca, Can; Fan, Wen; Luce, Alexander; Kang, Jeong Seuk; Liu, Jonathan; Ko, Changhyun; Raghunathanan, Rajamani; Zhou, Jian; Ogletree, Frank; Li, Jingbo; Grossman, Jeffrey C.; Wu, Junqiao

    2013-01-01

    Point defects in semiconductors can trap free charge carriers and localize excitons. The interaction between these defects and charge carriers becomes stronger at reduced dimensionalities, and is expected to greatly influence physical properties of the hosting material. We investigated effects of anion vacancies in monolayer transition metal dichalcogenides as two-dimensional (2D) semiconductors where the vacancies density is controlled by α-particle irradiation or thermal-annealing. We found a new, sub-bandgap emission peak as well as increase in overall photoluminescence intensity as a result of the vacancy generation. Interestingly, these effects are absent when measured in vacuum. We conclude that in opposite to conventional wisdom, optical quality at room temperature cannot be used as criteria to assess crystal quality of the 2D semiconductors. Our results not only shed light on defect and exciton physics of 2D semiconductors, but also offer a new route toward tailoring optical properties of 2D semiconductors by defect engineering. PMID:24029823

  15. The identification and nature of bound exciton I-line PL systems in ZnO

    Energy Technology Data Exchange (ETDEWEB)

    Johnston, K. [PH Dept, CERN, 1211-Geneva (Switzerland); Cullen, J.; Henry, M. O.; McGlynn, Enda [School of Physics Sciences, Dublin City University, Dublin 9 (Ireland); Khawaga, Rehab I. [Department of Chemistry, College of Art and Science, American University of Sharjah (AUS) (United Arab Emirates)

    2013-12-04

    The chemical identification of donor bound excitons in ZnO has been studied using radioactive ions. Implantations of {sup 117}Ag - which decays to radioactive Cd and In - have enabled the identification of the I{sub 2} optical feature as being the ionized donor counterpart of I{sub 9}, one of the most prominent optical features in the photoluminescence spectrum of ZnO. Both of these lines are consistent with In occupying a Zn site.

  16. Quasi-particle energies and optical excitations of ZnS monolayer honeycomb structure

    Energy Technology Data Exchange (ETDEWEB)

    Shahrokhi, Masoud, E-mail: shahrokhimasoud37@gmail.com

    2016-12-30

    Highlights: • The electronic and optical properties of ZnS honeycomb sheet are investigated. • The electronic properties were analyzed at three levels of GW approach. • The optical properties of these materials are investigated using the BSE approach. • Optical properties of ZnS sheet strongly dominated by excitonic effects. • Spectrum is dominated by strongly bound Frenkel excitons. - Abstract: Using ab-initio density functional theory calculations combined with many-body perturbation formalism we carried out the electronic structure and optical properties of 2D graphene-like ZnS structure. The electronic properties were analyzed at three levels of many-body GW approach (G{sub 0}W{sub 0}, GW{sub 0} and GW) constructed over a Generalized Gradient Approximation functional. Our results indicate that ZnS sheet has a direct band gap at the Γ-point. Also it is seen that inclusion of electron–electron interaction does not change the sort of direct semiconducting band gap in ZnS sheet. The optical properties and excitonic effects of these materials are investigated using the Bethe-Salpeter equation (BSE) approach. The formation of first exciton peaks at 3.86, 4.26, and 4.57 eV with large binding energy of 0.36, 0.49 and 0.73 eV using G{sub 0}W{sub 0} + BSE, GW{sub 0} + BSE and GW + BSE, respectively, was observed. We show that the optical absorption spectrum of 2D ZnS structure is dominated by strongly bound Frenkel excitons. The enhanced excitonic effects in the ZnS monolayer sheet can be useful in designing optoelectronic applications.

  17. Trapping time of excitons in Si nanocrystals embedded in a SiO2 matrix

    Science.gov (United States)

    de Jong, E. M. L. D.; de Boer, W. D. A. M.; Yassievich, I. N.; Gregorkiewicz, T.

    2017-05-01

    Silicon (Si) nanocrystals (NCs) are of great interest for many applications, ranging from photovoltaics to optoelectonics. The photoluminescence quantum yield of Si NCs dispersed in SiO2 is limited, suggesting the existence of very efficient processes of nonradiative recombination, among which the formation of a self-trapped exciton state on the surface of the NC. In order to improve the external quantum efficiency of these systems, the carrier relaxation and recombination need to be understood more thoroughly. For that purpose, we perform transient-induced absorption spectroscopy on Si NCs embedded in a SiO2 matrix over a broad probe range for NCs of average sizes from 2.5 to 5.5 nm. The self-trapping of free excitons on surface-related states is experimentally and theoretically discussed and found to be dependent on the NC size. These results offer more insight into the self-trapped exciton state and are important to increase the optical performance of Si NCs.

  18. Dependence of Exciton Diffusion Length and Diffusion Coefficient on Photophysical Parameters in Bulk Heterojunction Organic Solar Cells

    Science.gov (United States)

    Yeboah, Douglas; Singh, Jai

    2017-11-01

    Recently, the dependence of exciton diffusion length (LD ) on some photophysical parameters of organic solids has been experimentally demonstrated, however no systematic theoretical analysis of this phenomenon has been carried out. We have conducted a theoretical study by using the Förster resonance energy transfer and Dexter carrier transfer mechanisms together with the Einstein-Smoluchowski diffusion equation to derive analytical models for the diffusion lengths (LD ) and diffusion coefficients (D) of singlet (S) and triplet (T) excitons in organic solids as functions of spectral overlap integral (J) , photoluminescence (PL) quantum yield (φD ) , dipole moment (μT ) and refractive index (n) of the photoactive material. The exciton diffusion lengths and diffusion coefficients in some selected organic solids were calculated, and we found that the singlet exciton diffusion length (LDS ) increases with φD and J, and decreases with n. Also, the triplet exciton diffusion length (LDT ) increases with φD and decreases with μT . These may be achieved through doping the organic solids into broad optical energy gap host materials as observed in previous experiments. The calculated exciton diffusion lengths are compared with experimental values and a reasonably good agreement is found between them. The results presented are expected to provide insight relevant to the synthesis of new organic solids for fabrication of bulk heterojunction organic solar cells characterized by better power conversion efficiency.

  19. Exciton-dopant and exciton-charge interactions in electronically doped OLEDs

    International Nuclear Information System (INIS)

    Williams, Christopher; Lee, Sergey; Ferraris, John; Zakhidov, A. Anvar

    2004-01-01

    The electronic dopants, like tetrafluorocyanoquinodimethane (F 4 -TCNQ) molecules, used for p-doping of hole transport layers in organic light-emitting diodes (OLEDs) are found to quench the electroluminescence (EL) if they diffuse into the emissive layer. We observed EL quenching in OLED with F 4 -TCNQ doped N,N'-diphenyl-N'N'-bis(1-naphthyl)-1,1'-biphenyl-4,4'-diamine hole transport layer at large dopant concentrations, >5%. To separate the effects of exciton-dopant quenching, from exciton-polaron quenching we have intentionally doped the emissive layer of (8-tris-hydroxyquinoline) with three acceptors (A) of different electron affinities: F 4 -TCNQ, TCNQ, and C 60 , and found that C 60 is the strongest EL-quencher, while F 4 -TCNQ is the weakest, contrary to intuitive expectations. The new effects of charge transfer and usually considered energy transfer from exciton to neutral (A) and charged acceptors (A - ) are compared as channels for non-radiative Ex-A decay. At high current loads the EL quenching is observed, which is due to decay of Ex on free charge carriers, hole polarons P + . We consider contributions to Ex-P + interaction by short-range charge transfer and describe the structure of microscopic charge transfer (CT)-processes responsible for it. The formation of metastable states of 'charged excitons' (predicted and studied by Agranovich et al. Chem. Phys. 272 (2001) 159) by electron transfer from a P to an Ex is pointed out, and ways to suppress non-radiative Ex-P decay are suggested

  20. Exciton-polaritons in cuprous oxide: Theory and comparison with experiment

    Science.gov (United States)

    Schweiner, Frank; Ertl, Jan; Main, Jörg; Wunner, Günter; Uihlein, Christoph

    2017-12-01

    The observation of giant Rydberg excitons in cuprous oxide (Cu2O ) up to a principal quantum number of n =25 by T. Kazimierczuk et al. [Nature (London) 514, 343 (2014), 10.1038/nature13832] inevitably raises the question whether these quasiparticles must be described within a multipolariton framework since excitons and photons are always coupled in the solid. In this paper we present the theory of exciton-polaritons in Cu2O . To this end we extend the Hamiltonian which includes the complete valence-band structure, the exchange interaction, and the central-cell corrections effects, and which has been recently deduced by F. Schweiner et al. [Phys. Rev. B 95, 195201 (2017), 10.1103/PhysRevB.95.195201], for finite values of the exciton momentum ℏ K . We derive formulas to calculate not only dipole but also quadrupole oscillator strengths when using the complete basis of F. Schweiner et al., which has recently been proven as a powerful tool to calculate exciton spectra. Very complex polariton spectra for the three orientations of K along the axes [001 ] , [110 ] , and [111 ] of high symmetry are obtained and a strong mixing of exciton states is reported. The main focus is on the 1 S ortho-exciton-polariton, for which pronounced polariton effects have been measured in experiments. We set up a 5 ×5 matrix model, which accounts for both the polariton effect and the K -dependent splitting, and which allows treating the anisotropic polariton dispersion for any direction of K . We especially discuss the dispersions for K being oriented in the planes perpendicular to [1 1 ¯0 ] and [111 ] , for which experimental transmission spectra have been measured. Furthermore, we compare our results with experimental values of the K -dependent splitting, the group velocity, and the oscillator strengths of this exciton-polariton. The results are in good agreement. This proves the validity of the 5 ×5 matrix model as a useful theoretical model for further investigations on the 1 S

  1. Exciton Formation in Disordered Semiconductors

    DEFF Research Database (Denmark)

    Klochikhin, A.; Reznitsky, A.; Permogorov, S.

    1999-01-01

    Stationary luminescence spectra of disordered solid solutions can be accounted by the model of localized excitons. Detailed analysis of the long time decay kinetics of luminescence shows that exciton formation in these systems is in great extent due to the bimolecular reaction of separated carrie...

  2. Symmetry and optical anisotropy in CdSe/ZnSe quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Kiessling, Tobias

    2009-10-29

    The material system of choice for the investigations performed in the frame of this Thesis were self-assembled CdSe/ZnSe QDs. The reason for this choice is twofold. First, CdSe/ZnSe QDs can be grown with excellent optical quality, which is a prerequiste for optical studies. Second, due to the polar nature of II-VI compound semiconductors, optical anisotropies induced by various asymmetries are more pronounced than in their IIIV or element IV counterparts. Unlike in the III-V materials, where the self-organization of QDs is well described by the Stranski-Krastanow growth mode, the peculiarities of the QD formation are not entirely clear in II-VI alloys. For the purposes of the current work QDs emerging from two variants of Molecular Beam Epitaxy (MBE) growth were studied. In order to establish a clear connection between the optically observed anisotropies and the growth induced asymmetries in the QDs we start out by summarizing all available structural and morphological studies that were performed on the resultant QDs, including x-ray diffraction, atomic force microscopy, high resolution transmission electron microscopy and resonant Raman scattering. Extensive investigations by Photoluminescence (PL) and Photoluminescence Excitation (PLE) spectroscopy hence detail the resultant electronic structure of excitons confined to the above QDs as well as their energy relaxation across the latter. We find that for these small-sized strongly confining QDs k-vector conservation is entirely relaxed, which enables interaction of the excitons with a continuum of phonons and explains fast and efficient exciton capture by the QDs, even for excitation conditions far above the ground state. We demonstrate how this provides an alternative fast relaxation channel to Auger-like electron-hole scattering, that may also explain fast hole relaxation and adds to the understanding of the absence of a phonon bottleneck in the energy relaxation in these type of QDs. With the above analysis as a

  3. Symmetry and optical anisotropy in CdSe/ZnSe quantum dots

    International Nuclear Information System (INIS)

    Kiessling, Tobias

    2009-01-01

    The material system of choice for the investigations performed in the frame of this Thesis were self-assembled CdSe/ZnSe QDs. The reason for this choice is twofold. First, CdSe/ZnSe QDs can be grown with excellent optical quality, which is a prerequiste for optical studies. Second, due to the polar nature of II-VI compound semiconductors, optical anisotropies induced by various asymmetries are more pronounced than in their IIIV or element IV counterparts. Unlike in the III-V materials, where the self-organization of QDs is well described by the Stranski-Krastanow growth mode, the peculiarities of the QD formation are not entirely clear in II-VI alloys. For the purposes of the current work QDs emerging from two variants of Molecular Beam Epitaxy (MBE) growth were studied. In order to establish a clear connection between the optically observed anisotropies and the growth induced asymmetries in the QDs we start out by summarizing all available structural and morphological studies that were performed on the resultant QDs, including x-ray diffraction, atomic force microscopy, high resolution transmission electron microscopy and resonant Raman scattering. Extensive investigations by Photoluminescence (PL) and Photoluminescence Excitation (PLE) spectroscopy hence detail the resultant electronic structure of excitons confined to the above QDs as well as their energy relaxation across the latter. We find that for these small-sized strongly confining QDs k-vector conservation is entirely relaxed, which enables interaction of the excitons with a continuum of phonons and explains fast and efficient exciton capture by the QDs, even for excitation conditions far above the ground state. We demonstrate how this provides an alternative fast relaxation channel to Auger-like electron-hole scattering, that may also explain fast hole relaxation and adds to the understanding of the absence of a phonon bottleneck in the energy relaxation in these type of QDs. With the above analysis as a

  4. Fractional Solitons in Excitonic Josephson Junctions

    OpenAIRE

    Hsu, Ya-Fen; Su, Jung-Jung

    2015-01-01

    The Josephson effect is especially appealing to physicists because it reveals macroscopically the quantum order and phase. In excitonic bilayers the effect is even subtler due to the counterflow of supercurrent as well as the tunneling between layers (interlayer tunneling). Here we study, in a quantum Hall bilayer, the excitonic Josephson junction: a conjunct of two exciton condensates with a relative phase ? 0 applied. The system is mapped into a pseudospin ferromagnet then described numeric...

  5. Semiconductor quantum optics with tailored photonic nanostructures

    Energy Technology Data Exchange (ETDEWEB)

    Laucht, Arne

    2011-06-15

    This thesis describes detailed investigations of the effects of photonic nanostructures on the light emission properties of self-assembled InGaAs quantum dots. Nanoscale optical cavities and waveguides are employed to enhance the interaction between light and matter, i.e. photons and excitons, up to the point where optical non-linearities appear at the quantum (single photon) level. Such non-linearities are an essential component for the realization of hardware for photon based quantum computing since they can be used for the creation and detection of non-classical states of light and may open the way to new genres of quantum optoelectronic devices such as optical modulators and optical transistors. For single semiconductor quantum dots in photonic crystal nanocavities we investigate the coupling between excitonic transitions and the highly localized mode of the optical cavity. We explore the non-resonant coupling mechanisms which allow excitons to couple to the cavity mode, even when they are not spectrally in resonance. This effect is not observed for atomic cavity quantum electrodynamics experiments and its origin is traced to phonon-assisted scattering for small detunings ({delta}E<{proportional_to}5 meV) and a multi-exciton-based, Auger-like process for larger detunings ({delta}E >{proportional_to}5 meV). For quantum dots in high-Q cavities we observe the coherent coupling between exciton and cavity mode in the strong coupling regime of light-matter interaction, probe the influence of pure dephasing on the coherent interaction at high excitation levels and high lattice temperatures, and examine the coupling of two spatially separated quantum dots via the exchange of real and virtual photons mediated by the cavity mode. Furthermore, we study the spontaneous emission properties of quantum dots in photonic crystal waveguide structures, estimate the fraction of all photons emitted into the propagating waveguide mode, and demonstrate the on-chip generation of

  6. Chiral topological excitons in a Chern band insulator

    Science.gov (United States)

    Chen, Ke; Shindou, Ryuichi

    2017-10-01

    A family of semiconductors called Chern band insulators are shown to host exciton bands with nonzero topological Chern integers and chiral exciton edge modes. Using a prototypical two-band Chern insulator model, we calculate a cross-correlation function to obtain the exciton bands and their Chern integers. The lowest exciton band acquires Chern integers such as ±1 and ±2 in the electronic Chern insulator phase. The nontrivial topology can be experimentally observed both by a nonlocal optoelectronic response of exciton edge modes and by a phase shift in the cross-correlation response due to the bulk mode. Our result suggests that magnetically doped HgTe, InAs/GaSb quantum wells, and (Bi,Sb)2Te3 thin films are promising candidates for a platform of topological excitonics.

  7. Preface to the SPECIAL ISSUE: Excitonic Solar Cells(II)

    Institute of Scientific and Technical Information of China (English)

    Jianjun Tian; Meicheng Li; Kaibo Zheng

    2016-01-01

    Among all the excitonic solar cells(ESCs)including dyesensitized solar cells(DSSCs),quantum solar cells(QDSCs),perovskites solar cells(PSCs),and organic photovoltaics(OPVs),PSCs attracted enormous research attention in the past 7 years and attained the highest power conversion efficiency(PCE)of over 20%with the biggest progress,from 3.8%to over 22.1%in 7 years.However,one can easily realize the fact that such a rapid progress achieved in PSCs was made possible is largely based on the fundamental knowledge,experimental skills,and characterization facilities obtained and accumulated through the multi-decade long endeavor in the study of other excitonic solar cells.Even though PSCs have attractedmuch research human resource and funding,the study on other excitonic solar cells has never stopped,and such persistent efforts

  8. Highly Anisotropic in-Plane Excitons in Atomically Thin and Bulklike 1T '-ReSe2

    DEFF Research Database (Denmark)

    Arora, Ashish; Noky, Jonathan; Drueppel, Matthias

    2017-01-01

    and photoluminescence spectroscopy of excitons in 1T '-ReSe2. On reducing the crystal thickness from bulk to a monolayer, we observe a strong blue shift of the optical band gap from 1.37 to 1.50 eV. The excitons are strongly polarized with dipole vectors along different crystal directions, which persist from bulk down......Atomically thin materials such as graphene or MoS2 are of high in-plane symmetry. Crystals with reduced symmetry hold the promise for novel optoelectronic devices based on their anisotropy in current flow or light polarization. Here, we present polarization-resolved optical transmission...... crystal. In addition, we find in our calculations a direct band gap in 1T '-ReSe2 regardless of crystal thickness, indicating weak interlayer coupling effects on the band gap characteristics. Our results pave the way for polarization-sensitive applications, such as optical logic circuits operating...

  9. Simulation of excitonic optical line shapes of cyclic oligomers - models for basic units of photosynthetic antenna systems: Transfer integral versus local energy fluctuations with dichotomic coloured noise

    International Nuclear Information System (INIS)

    Barvik, I.; Reineker, P.; Warns, C.; Neidlinger, T.

    1995-08-01

    For Frenkel excitons moving on cyclic and linear molecular chains modeling in part photosynthetic antenna systems we investigate the influence of dynamic and static disorder on their optical line shapes. The dynamic disorder describes the influence of vibrational degrees of freedom and is taken into account by fluctuations of the transfer matrix element between neighbouring molecules. The fluctuations are represented by dichotomic Markov processes with coloured noise. We obtain a closed set of equations of motion for the correlation functions determining the optical line shape which is solved exactly. The line shapes are discussed for various sets of the model parameters and arrangements of molecules and their dipole moments. (author). 63 refs, 10 figs

  10. Instantaneous Rayleigh scattering from excitons localized in monolayer islands

    DEFF Research Database (Denmark)

    Langbein, Wolfgang; Leosson, Kristjan; Jensen, Jacob Riis

    2000-01-01

    We show that the initial dynamics of Rayleigh scattering from excitons in quantum wells can be either instantaneous or delayed, depending on the exciton ensemble studied. For excitation of the entire exciton resonance, a finite rise time given by the inverse inhomogeneous broadening: of the exciton...

  11. Anisotropy of exciton spectrum and spin-orbit interactions in quantum wells in tilted magnetic field

    International Nuclear Information System (INIS)

    Olendski, Oleg; Shahbazyan, Tigran V

    2006-01-01

    We study theoretically excitonic energy spectrum and optical absorption in narrowgap semiconductor quantum wells in strong magnetic field. We show that, in the presence of an in-plane field component, the absorption coefficient exhibit a double-peak structure due to hybridization of bright and dark excitons. If both Rashba and Dresselhaus spin-orbit terms are present, the spectrum is anisotropic in in-plane field orientation with respect to [100] axis. In particular, the magnitude of the splitting can be tuned in a wide interval by varying the azimuthal angle of the in-plane field. The absorption spectrrum anisotropy would allow simultaneous measurement Dresselhaus and Rashba spin-orbit coefficients

  12. Excitonic recombination dynamics in non-polar GaN/AlGaN quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Rosales, D.; Gil, B.; Bretagnon, T.; Guizal, B. [CNRS, Laboratoire Charles Coulomb, UMR 5221, F-34095 Montpellier (France); Université Montpellier 2, Laboratoire Charles Coulomb, UMR 5221, F-34095 Montpellier (France); Zhang, F.; Okur, S.; Monavarian, M.; Izyumskaya, N.; Avrutin, V.; Özgür, Ü.; Morkoç, H. [Department of Electrical and Computer Engineering, Virginia Commonwealth University, Richmond, Virginia 23238 (United States); Leach, J. H. [Kyma Technologies, Raleigh, North Carolina 27617 (United States)

    2014-02-21

    The optical properties of GaN/Al{sub 0.15}Ga{sub 0.85}N multiple quantum wells are examined in 8 K–300 K temperature range. Both polarized CW and time resolved temperature-dependent photoluminescence experiment are performed so that we can deduce the relative contributions of the non-radiative and radiative recombination processes. From the calculation of the proportion of the excitonic population having wave vector in the light cone, we can deduce the variation of the radiative decay time with temperature. We find part of the excitonic population to be localized in concert with the report of Corfdir et al. (Jpn. J. Appl. Phys., Part 2 52, 08JC01 (2013)) in case of a-plane quantum wells.

  13. Excitonic recombination dynamics in non-polar GaN/AlGaN quantum wells

    International Nuclear Information System (INIS)

    Rosales, D.; Gil, B.; Bretagnon, T.; Guizal, B.; Zhang, F.; Okur, S.; Monavarian, M.; Izyumskaya, N.; Avrutin, V.; Özgür, Ü.; Morkoç, H.; Leach, J. H.

    2014-01-01

    The optical properties of GaN/Al 0.15 Ga 0.85 N multiple quantum wells are examined in 8 K–300 K temperature range. Both polarized CW and time resolved temperature-dependent photoluminescence experiment are performed so that we can deduce the relative contributions of the non-radiative and radiative recombination processes. From the calculation of the proportion of the excitonic population having wave vector in the light cone, we can deduce the variation of the radiative decay time with temperature. We find part of the excitonic population to be localized in concert with the report of Corfdir et al. (Jpn. J. Appl. Phys., Part 2 52, 08JC01 (2013)) in case of a-plane quantum wells

  14. Exciton fission in monolayer transition metal dichalcogenide semiconductors.

    Science.gov (United States)

    Steinhoff, A; Florian, M; Rösner, M; Schönhoff, G; Wehling, T O; Jahnke, F

    2017-10-27

    When electron-hole pairs are excited in a semiconductor, it is a priori not clear if they form a plasma of unbound fermionic particles or a gas of composite bosons called excitons. Usually, the exciton phase is associated with low temperatures. In atomically thin transition metal dichalcogenide semiconductors, excitons are particularly important even at room temperature due to strong Coulomb interaction and a large exciton density of states. Using state-of-the-art many-body theory, we show that the thermodynamic fission-fusion balance of excitons and electron-hole plasma can be efficiently tuned via the dielectric environment as well as charge carrier doping. We propose the observation of these effects by studying exciton satellites in photoemission and tunneling spectroscopy, which present direct solid-state counterparts of high-energy collider experiments on the induced fission of composite particles.

  15. Nonlinear optics response of semiconductor quantum wells under high magnetic fields

    International Nuclear Information System (INIS)

    Chemla, D.S.

    1993-07-01

    Recent investigations on the nonlinear optical response of semiconductor quantum wells in a strong perpendicular magnetic field, H, are reviewed. After some introductory material the evolution of the linear optical properties of GaAs QW's as a function of H is discussed; an examination is made of how the magneto-excitons (MX) extrapolate continuously between quasi-2D QW excitons (X) when H = 0, and pairs of Landau levels (LL) when H → ∞. Next, femtosecond time resolved investigations of their nonlinear optical response are presented; the evolution of MX-MX interactions with increasing H is stressed. Finally, how, as the dimensionality is reduced by application of H, the number of scattering channels is limited and relaxation of electron-hole pairs is affected. How nonlinear optical spectroscopy can be exploited to access the relaxation of angular momentum within magneto-excitons is also discussed

  16. Chiral Modes at Exceptional Points in Exciton-Polariton Quantum Fluids

    Science.gov (United States)

    Gao, T.; Li, G.; Estrecho, E.; Liew, T. C. H.; Comber-Todd, D.; Nalitov, A.; Steger, M.; West, K.; Pfeiffer, L.; Snoke, D. W.; Kavokin, A. V.; Truscott, A. G.; Ostrovskaya, E. A.

    2018-02-01

    We demonstrate the generation of chiral modes-vortex flows with fixed handedness in exciton-polariton quantum fluids. The chiral modes arise in the vicinity of exceptional points (non-Hermitian spectral degeneracies) in an optically induced resonator for exciton polaritons. In particular, a vortex is generated by driving two dipole modes of the non-Hermitian ring resonator into degeneracy. Transition through the exceptional point in the space of the system's parameters is enabled by precise manipulation of real and imaginary parts of the closed-wall potential forming the resonator. As the system is driven to the vicinity of the exceptional point, we observe the formation of a vortex state with a fixed orbital angular momentum (topological charge). This method can be extended to generate higher-order orbital angular momentum states through coalescence of multiple non-Hermitian spectral degeneracies. Our Letter demonstrates the possibility of exploiting nontrivial and counterintuitive properties of waves near exceptional points in macroscopic quantum systems.

  17. Chiral Modes at Exceptional Points in Exciton-Polariton Quantum Fluids.

    Science.gov (United States)

    Gao, T; Li, G; Estrecho, E; Liew, T C H; Comber-Todd, D; Nalitov, A; Steger, M; West, K; Pfeiffer, L; Snoke, D W; Kavokin, A V; Truscott, A G; Ostrovskaya, E A

    2018-02-09

    We demonstrate the generation of chiral modes-vortex flows with fixed handedness in exciton-polariton quantum fluids. The chiral modes arise in the vicinity of exceptional points (non-Hermitian spectral degeneracies) in an optically induced resonator for exciton polaritons. In particular, a vortex is generated by driving two dipole modes of the non-Hermitian ring resonator into degeneracy. Transition through the exceptional point in the space of the system's parameters is enabled by precise manipulation of real and imaginary parts of the closed-wall potential forming the resonator. As the system is driven to the vicinity of the exceptional point, we observe the formation of a vortex state with a fixed orbital angular momentum (topological charge). This method can be extended to generate higher-order orbital angular momentum states through coalescence of multiple non-Hermitian spectral degeneracies. Our Letter demonstrates the possibility of exploiting nontrivial and counterintuitive properties of waves near exceptional points in macroscopic quantum systems.

  18. Direct measurement of exciton valley coherence in monolayer WSe2

    KAUST Repository

    Hao, Kai

    2016-02-29

    In crystals, energy band extrema in momentum space can be identified by a valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier, analogous to electronic charge or spin. Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition metal dichalcogenides. However, the valley coherence time—a crucial quantity for valley pseudospin manipulation—is difficult to directly probe. In this work, we use two-dimensional coherent spectroscopy to resonantly generate and detect valley coherence of excitons (Coulomb-bound electron–hole pairs) in monolayer WSe2 (refs ,). The imposed valley coherence persists for approximately one hundred femtoseconds. We propose that the electron–hole exchange interaction provides an important decoherence mechanism in addition to exciton population recombination. This work provides critical insight into the requirements and strategies for optical manipulation of the valley pseudospin for future valleytronics applications.

  19. Acousto-exciton interaction in a gas of 2D indirect dipolar excitons in the presence of disorder

    Energy Technology Data Exchange (ETDEWEB)

    Kovalev, V. M.; Chaplik, A. V., E-mail: chaplik@isp.nsc.ru [Russian Academy of Sciences, Rzhanov Institute of Semiconductor Physics, Siberian Branch (Russian Federation)

    2016-03-15

    A theory for the linear and quadratic responses of a 2D gas of indirect dipolar excitons to an external surface acoustic wave perturbation in the presence of a static random potential is considered. The theory is constructed both for high temperatures, definitely greater than the exciton gas condensation temperature, and at zero temperature by taking into account the Bose–Einstein condensation effects. The particle Green functions, the density–density correlation function, and the quadratic response function are calculated by the “cross” diagram technique. The results obtained are used to calculate the absorption of Rayleigh surface waves and the acoustic exciton gas drag by a Rayleigh wave. The damping of Bogoliubov excitations in an exciton condensate due to theirs scattering by a random potential has also been determined.

  20. Electrons, holes, and excitons in GaAs polytype quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Climente, Juan I.; Segarra, Carlos; Rajadell, Fernando; Planelles, Josep, E-mail: josep.planelles@uji.es [Departament de Química Física i Analítica, Universitat Jaume I, E-12080 Castelló (Spain)

    2016-03-28

    Single and multi-band k⋅p Hamiltonians for GaAs crystal phase quantum dots are used to assess ongoing experimental activity on the role of such factors as quantum confinement, spontaneous polarization, valence band mixing, and exciton Coulomb interaction. Spontaneous polarization is found to be a dominating term. Together with the control of dot thickness [Vainorius et al., Nano Lett. 15, 2652 (2015)], it enables wide exciton wavelength and lifetime tunability. Several new phenomena are predicted for small diameter dots [Loitsch et al., Adv. Mater. 27, 2195 (2015)], including non-heavy hole ground state, strong hole spin admixture, and a type-II to type-I exciton transition, which can be used to improve the absorption strength and reduce the radiative lifetime of GaAs polytypes.

  1. Semiconductor quantum optics with tailored photonic nanostructures

    International Nuclear Information System (INIS)

    Laucht, Arne

    2011-01-01

    This thesis describes detailed investigations of the effects of photonic nanostructures on the light emission properties of self-assembled InGaAs quantum dots. Nanoscale optical cavities and waveguides are employed to enhance the interaction between light and matter, i.e. photons and excitons, up to the point where optical non-linearities appear at the quantum (single photon) level. Such non-linearities are an essential component for the realization of hardware for photon based quantum computing since they can be used for the creation and detection of non-classical states of light and may open the way to new genres of quantum optoelectronic devices such as optical modulators and optical transistors. For single semiconductor quantum dots in photonic crystal nanocavities we investigate the coupling between excitonic transitions and the highly localized mode of the optical cavity. We explore the non-resonant coupling mechanisms which allow excitons to couple to the cavity mode, even when they are not spectrally in resonance. This effect is not observed for atomic cavity quantum electrodynamics experiments and its origin is traced to phonon-assisted scattering for small detunings (ΔE ∝5 meV). For quantum dots in high-Q cavities we observe the coherent coupling between exciton and cavity mode in the strong coupling regime of light-matter interaction, probe the influence of pure dephasing on the coherent interaction at high excitation levels and high lattice temperatures, and examine the coupling of two spatially separated quantum dots via the exchange of real and virtual photons mediated by the cavity mode. Furthermore, we study the spontaneous emission properties of quantum dots in photonic crystal waveguide structures, estimate the fraction of all photons emitted into the propagating waveguide mode, and demonstrate the on-chip generation of single photon emission into the waveguide. The results obtained during the course of this thesis contribute significantly to

  2. Magnetic field effect on the energy levels of an exciton in a GaAs quantum dot: Application for excitonic lasers.

    Science.gov (United States)

    Jahan, K Luhluh; Boda, A; Shankar, I V; Raju, Ch Narasimha; Chatterjee, Ashok

    2018-03-22

    The problem of an exciton trapped in a Gaussian quantum dot (QD) of GaAs is studied in both two and three dimensions in the presence of an external magnetic field using the Ritz variational method, the 1/N expansion method and the shifted 1/N expansion method. The ground state energy and the binding energy of the exciton are obtained as a function of the quantum dot size, confinement strength and the magnetic field and compared with those available in the literature. While the variational method gives the upper bound to the ground state energy, the 1/N expansion method gives the lower bound. The results obtained from the shifted 1/N expansion method are shown to match very well with those obtained from the exact diagonalization technique. The variation of the exciton size and the oscillator strength of the exciton are also studied as a function of the size of the quantum dot. The excited states of the exciton are computed using the shifted 1/N expansion method and it is suggested that a given number of stable excitonic bound states can be realized in a quantum dot by tuning the quantum dot parameters. This can open up the possibility of having quantum dot lasers using excitonic states.

  3. Directing energy transport in organic photovoltaic cells using interfacial exciton gates.

    Science.gov (United States)

    Menke, S Matthew; Mullenbach, Tyler K; Holmes, Russell J

    2015-04-28

    Exciton transport in organic semiconductors is a critical, mediating process in many optoelectronic devices. Often, the diffusive and subdiffusive nature of excitons in these systems can limit device performance, motivating the development of strategies to direct exciton transport. In this work, directed exciton transport is achieved with the incorporation of exciton permeable interfaces. These interfaces introduce a symmetry-breaking imbalance in exciton energy transfer, leading to directed motion. Despite their obvious utility for enhanced exciton harvesting in organic photovoltaic cells (OPVs), the emergent properties of these interfaces are as yet uncharacterized. Here, directed exciton transport is conclusively demonstrated in both dilute donor and energy-cascade OPVs where judicious optimization of the interface allows exciton transport to the donor-acceptor heterojunction to occur considerably faster than when relying on simple diffusion. Generalized systems incorporating multiple exciton permeable interfaces are also explored, demonstrating the ability to further harness this phenomenon and expeditiously direct exciton motion, overcoming the diffusive limit.

  4. 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

  5. Optical and electronic properties of InGaAs and nitride quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Baer, N.

    2006-06-15

    In the present thesis, the electronic and optical properties of such nanostructures have been investigated for the well established III-V and the new group-III nitride material system. The influence of Coulomb correlations on the optical spectra of InGaAs QDs are studied using a full configuration interaction approach. The resulting multi-exciton spectra for up to twelve excitons are investigated in detail. Characteristic features of the spectra are explained using simplified Hamiltonians that are derived taking into account the relative importance of various interaction contributions. Additionally, we study the electronic and optical properties of self-assembled InN/GaN quantum dots. The existence of an exactly degenerate p-shell is discussed in detail. Dipole and Coulomb matrix elements are calculated from these one-particle wave functions and serve as an input for configuration interaction calculations. We present multi-exciton emission spectra and investigate how Coulomb correlations and oscillator strengths are altered by the built-in electrostatic fields present in these structures. From our results, we predict vanishing exciton and biexciton ground state emission for small lens-shaped dots, which is explained by a careful analysis of the underlying symmetry group. To study the photoluminescence dynamics of an initially excited QD system, we employ a microscopic semiconductor theory. Carrier-carrier correlations beyond the Hartee-Fock level are included within a cluster expansion truncation scheme up to the singlet-doublet level. The influence of these correlations on the spectrum and the photoluminescence dynamics is investigated for the emission into free space as well as for QDs embedded in an optical microcavity. (orig.)

  6. Optical and electronic properties of InGaAs and nitride quantum dots

    International Nuclear Information System (INIS)

    Baer, N.

    2006-06-01

    In the present thesis, the electronic and optical properties of such nanostructures have been investigated for the well established III-V and the new group-III nitride material system. The influence of Coulomb correlations on the optical spectra of InGaAs QDs are studied using a full configuration interaction approach. The resulting multi-exciton spectra for up to twelve excitons are investigated in detail. Characteristic features of the spectra are explained using simplified Hamiltonians that are derived taking into account the relative importance of various interaction contributions. Additionally, we study the electronic and optical properties of self-assembled InN/GaN quantum dots. The existence of an exactly degenerate p-shell is discussed in detail. Dipole and Coulomb matrix elements are calculated from these one-particle wave functions and serve as an input for configuration interaction calculations. We present multi-exciton emission spectra and investigate how Coulomb correlations and oscillator strengths are altered by the built-in electrostatic fields present in these structures. From our results, we predict vanishing exciton and biexciton ground state emission for small lens-shaped dots, which is explained by a careful analysis of the underlying symmetry group. To study the photoluminescence dynamics of an initially excited QD system, we employ a microscopic semiconductor theory. Carrier-carrier correlations beyond the Hartee-Fock level are included within a cluster expansion truncation scheme up to the singlet-doublet level. The influence of these correlations on the spectrum and the photoluminescence dynamics is investigated for the emission into free space as well as for QDs embedded in an optical microcavity. (orig.)

  7. Spin-exciton interaction and related micro-photoluminescence spectra of ZnSe:Mn DMS nanoribbon.

    Science.gov (United States)

    Hou, Lipeng; Zhou, Weichang; Zou, Bingsuo; Zhang, Yu; Han, Junbo; Yang, Xinxin; Gong, Zhihong; Li, Jingbo; Xie, Sishen; Shi, Li-Jie

    2017-03-10

    For their spintronic applications the magnetic and optical properties of diluted magnetic semiconductors (DMS) have been studied widely. However, the exact relationships between the magnetic interactions and optical emission behaviors in DMS are not well understood yet due to their complicated microstructural and compositional characters from different growth and preparation techniques. Manganese (Mn) doped ZnSe nanoribbons with high quality were obtained by using the chemical vapor deposition (CVD) method. Successful Mn ion doping in a single ZnSe nanoribbon was identified by elemental energy-dispersive x-ray spectroscopy mapping and micro-photoluminescence (PL) mapping of intrinsic d-d optical transition at 580 nm, i.e. the transition of 4 T 1 ( 4 G) →  6 A 1 ( 6 s),. Besides the d-d transition PL peak at 580 nm, two other PL peaks related to Mn ion aggregates in the ZnSe lattice were detected at 664 nm and 530 nm, which were assigned to the d-d transitions from the Mn 2+ -Mn 2+ pairs with ferromagnetic (FM) coupling and antiferromagnetic (AFM) coupling, respectively. Moreover, AFM pair formation goes along with strong coupling with acoustic phonon or structural defects. These arguments were supported by temperature-dependent PL spectra, power-dependent PL lifetimes, and first-principle calculations. Due to the ferromagnetic pair existence, an exciton magnetic polaron (EMP) is formed and emits at 460 nm. Defect existence favors the AFM pair, which also can account for its giant enhancement of spin-orbital coupling and the spin Hall effect observed in PRL 97, 126603(2006) and PRL 96, 196404(2006). These emission results of DMS reflect their relation to local sp-d hybridization, spin-spin magnetic coupling, exciton-spin or phonon interactions covering structural relaxations. This kind of material can be used to study the exciton-spin interaction and may find applications in spin-related photonic devices besides spintronics.

  8. Effective exciton blocking by the hole-transporting material 5,10,15-tribenzyl-5H-diindolo[3,2-a:3′,2′-c]-carbazole (TBDI) in the tetraphenyldibenzoperiflanthene (DBP) based organic photovoltaic cells

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Jing; Yang, Fang [School of Materials Science and Engineering, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Key Laboratory of Advanced Display and System Applications, Ministry of Education, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Zheng, Yanqiong, E-mail: zhengyanqiong@shu.edu.cn [Key Laboratory of Advanced Display and System Applications, Ministry of Education, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Shanghai Engineering Research Center of Flat Panel Display, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Wei, Bin [Key Laboratory of Advanced Display and System Applications, Ministry of Education, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Shanghai Engineering Research Center of Flat Panel Display, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Zhang, Xiaowen [Guangxi Key Laboratory of Information Materials, Guilin University of Electronic Technology, 1 Jinji Road, Guilin 541004 (China); Zhang, Jianhua; Wang, Zixing [Key Laboratory of Advanced Display and System Applications, Ministry of Education, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Shanghai Engineering Research Center of Flat Panel Display, Shanghai University, P.O. Box 143, 149 Yanchang Rd., Shanghai 200072 (China); Pu, Wenhong; Yang, Changzhu [School of Environmental Science and Engineering, Huazhong University of Science and Technology, 1037 Luoyu Road, Wuhan 430074 (China)

    2015-12-01

    Graphical abstract: The hole-transporting materials of TBDI, NPB and TAPC were used as exciton blocking layer (EBL) in DBP based PHJs for successfully blocking the misdirected electrons. PHJ cell with TBDI showed an improvement of 36% in η{sub PCE} relative to the reference cell without any EBL, owing to enhanced optical electric field, stronger prevention of exciton quenching, and a smoother TBDI/DBP surface. - Highlights: • TBDI, NPB, and TAPC as exciton blocking layers (EBLs) all successfully improved the performance of DBP PHJs. • A highest η{sub PCE} improvement of 36% is obtained by TBDI EBL among the three EBLs. • Optical electric fields for the wavelength of 610 nm are significantly enhanced via inserting 10-nm EBLs. • PL spectra indicated stronger prevention of exciton quenching by TBDI. • AFM images suggested smoother donor/acceptor interface with TBDI EBL. - Abstract: To explore the novel application of the hole-transporting material (HTM) as exciton blocking layer (EBL) in small molecule organic photovoltaic (OPV) cells, we introduce a recently reported HTM, 5,10,15-tribenzyl-5H-diindolo[3,2-a:3′,2′-c]-carbazole (TBDI), and the other two traditional HTMs, N,N′-diphenyl-N,N′-bis(1-naphthyl)-1,1′-biphenyl-4,4′-diamine (NPB) and 1,1′-bis(di-4-tolylaminophenyl) cyclohexane (TAPC), to serve as EBLs in the tetraphenyldibenzoperiflanthene (DBP) based planar heterojunction cells. Due to the large band gap of these materials, the EBLs successfully block the misdirected electrons. The optimized devices including the EBLs of TBDI, NPB and TAPC achieve power conversion efficiency (η{sub PCE}) of 1.70%, 1.33%, and 1.33%, respectively, whereas the control device without any EBL shows a η{sub PCE} of only 1.25%. The optical simulation indicates that the maximum optical electric fields for the PHJs including 10-nm EBLs at the wavelength of 610 nm are significantly enhanced relative to that for the 20-nm DBP based control device. By impedance

  9. Optical properties of phosphorene

    International Nuclear Information System (INIS)

    Yang, Jiong; Lu Yuerui

    2017-01-01

    Phosphorene is a two-dimensional semiconductor with layers-dependent bandgap in the near-infrared range and it has attracted a great deal of attention due to its high anisotropy and carrier mobility. The highly anisotropic nature of phosphorene has been demonstrated through Raman and polarization photoluminescence measurements. Photoluminescence spectroscopy has also revealed the layers-dependent bandgap of phosphorene. Furthermore, due to the reduced dimensionality and screening in phosphorene, excitons and trions can stably exist at elevated temperatures and have large binding energies. The exciton and trion dynamics are thus detected by applying electrical bias or optical injection to the phosphorene system. Finally, various optical and optoelectronic applications based on phosphorene have been demonstrated and discussed. (topical reviews)

  10. Bright triplet excitons in caesium lead halide perovskites

    Science.gov (United States)

    Becker, Michael A.; Vaxenburg, Roman; Nedelcu, Georgian; Sercel, Peter C.; Shabaev, Andrew; Mehl, Michael J.; Michopoulos, John G.; Lambrakos, Samuel G.; Bernstein, Noam; Lyons, John L.; Stöferle, Thilo; Mahrt, Rainer F.; Kovalenko, Maksym V.; Norris, David J.; Rainò, Gabriele; Efros, Alexander L.

    2018-01-01

    Nanostructured semiconductors emit light from electronic states known as excitons. For organic materials, Hund’s rules state that the lowest-energy exciton is a poorly emitting triplet state. For inorganic semiconductors, similar rules predict an analogue of this triplet state known as the ‘dark exciton’. Because dark excitons release photons slowly, hindering emission from inorganic nanostructures, materials that disobey these rules have been sought. However, despite considerable experimental and theoretical efforts, no inorganic semiconductors have been identified in which the lowest exciton is bright. Here we show that the lowest exciton in caesium lead halide perovskites (CsPbX3, with X = Cl, Br or I) involves a highly emissive triplet state. We first use an effective-mass model and group theory to demonstrate the possibility of such a state existing, which can occur when the strong spin-orbit coupling in the conduction band of a perovskite is combined with the Rashba effect. We then apply our model to CsPbX3 nanocrystals, and measure size- and composition-dependent fluorescence at the single-nanocrystal level. The bright triplet character of the lowest exciton explains the anomalous photon-emission rates of these materials, which emit about 20 and 1,000 times faster than any other semiconductor nanocrystal at room and cryogenic temperatures, respectively. The existence of this bright triplet exciton is further confirmed by analysis of the fine structure in low-temperature fluorescence spectra. For semiconductor nanocrystals, which are already used in lighting, lasers and displays, these excitons could lead to materials with brighter emission. More generally, our results provide criteria for identifying other semiconductors that exhibit bright excitons, with potential implications for optoelectronic devices.

  11. Influence of fluctuating strain on exciton reflection spectra

    DEFF Research Database (Denmark)

    Skettrup, Torben

    1982-01-01

    The influence of an internal distribution of strain on the exciton reflection spectra is investigated. The resulting fluctuating optical constants give rise to a fluctuating phase of reflectivity. The standard deviation σ of these phase fluctuations is the quantity which can be observed...... to derive the dependence of the phase of reflectivity on the direction of the fluctuating optical axis. The results obtained for σ are compared with the experimental depolarization spectra of ZnO. The only fitting parameter is the common standard deviation of the strain components. It is found......, for example, between crossed polarizers or from ellipsometric measurements. Assuming the phase fluctuations to obey a Gaussian distribution, σ can be expressed in a simple way in terms of the degree of polarization or the depolarization of the reflected light. σ is then derived in terms of the standard...

  12. Modeling Temperature Dependent Singlet Exciton Dynamics in Multilayered Organic Nanofibers

    DEFF Research Database (Denmark)

    de Sousa, Leonardo Evaristo; de Oliveira Neto, Pedro Henrique; Kjelstrup-Hansen, Jakob

    2018-01-01

    Organic nanofibers have shown potential for application in optoelectronic devices because of the tunability of their optical properties. These properties are influenced by the electronic structure of the molecules that compose the nanofibers, but also by the behavior of the excitons generated...... dynamics in multilayered organic nanofibers. By simulating absorption and emission spectra, the possible Förster transitions are identified. Then, a Kinetic Monte Carlo (KMC) model is employed in combination with a genetic algorithm to theoretically reproduce time resolved photoluminescence measurements...

  13. Measurement of Exciton Binding Energy of Monolayer WS2

    Science.gov (United States)

    Chen, Xi; Zhu, Bairen; Cui, Xiaodong

    Excitonic effects are prominent in monolayer crystal of transition metal dichalcogenides (TMDCs) because of spatial confinement and reduced Coulomb screening. Here we use linear differential transmission spectroscopy and two-photon photoluminescence excitation spectroscopy (TP-PLE) to measure the exciton binding energy of monolayer WS2. Peaks for excitonic absorptions of the direct gap located at K valley of the Brillouin zone and transitions from multiple points near Γ point of the Brillouin zone, as well as trion side band are shown in the linear absorption spectra of WS2. But there is no gap between distinct excitons and the continuum of the interband transitions. Strong electron-phonon scattering, overlap of excitons around Γ point and the transfer of the oscillator strength from interband continuum to exciton states make it difficult to resolve the electronic interband transition edge even down to 10K. The gap between excited states of the band-edge exciton and the single-particle band is probed by TP-PLE measurements. And the energy difference between 1s exciton and the single-particle gap gives the exciton binding energy of monolayer WS2 to be about 0.71eV. The work is supported by Area of excellency (AoE/P-04/08), CRF of Hong Kong Research Grant Council (HKU9/CRF/13G) and SRT on New Materials of The University of Hong Kong.

  14. Pentacene Excitons in Strong Electric Fields.

    Science.gov (United States)

    Kuhnke, Klaus; Turkowski, Volodymyr; Kabakchiev, Alexander; Lutz, Theresa; Rahman, Talat S; Kern, Klaus

    2018-02-05

    Electroluminescence spectroscopy of organic semiconductors in the junction of a scanning tunneling microscope (STM) provides access to the polarizability of neutral excited states in a well-characterized molecular geometry. We study the Stark shift of the self-trapped lowest singlet exciton at 1.6 eV in a pentacene nanocrystal. Combination of density functional theory (DFT) and time-dependent DFT (TDDFT) with experiment allows for assignment of the observation to a charge-transfer (CT) exciton. Its charge separation is perpendicular to the applied field, as the measured polarizability is moderate and the electric field in the STM junction is strong enough to dissociate a CT exciton polarized parallel to the applied field. The calculated electric-field-induced anisotropy of the exciton potential energy surface will also be of relevance to photovoltaic applications. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  15. Exciton molecule in semiconductors by two-photon absorption

    International Nuclear Information System (INIS)

    Arya, K.; Hassan, A.R.

    1976-07-01

    Direct creation of bi-exciton states by two-photon absorption in direct gap semiconductors is investigated theoretically. A numerical application to the case of CuCl shows that the two-photon absorption coefficient for bi-excitonic transitions is larger than that for two-photon interband transitions by three orders of magnitude. It becomes comparable to that for one-photon excitonic transitions for available laser intensities. The main contribution to this enhancement of the absorption coefficient for the transitions to the bi-exciton states is found to be from the resonance effect

  16. Theoretical and computational studies of excitons in conjugated polymers

    Science.gov (United States)

    Barford, William; Bursill, Robert J.; Smith, Richard W.

    2002-09-01

    We present a theoretical and computational analysis of excitons in conjugated polymers. We use a tight-binding model of π-conjugated electrons, with 1/r interactions for large r. In both the weak-coupling limit (defined by W>>U) and the strong-coupling limit (defined by Wparticle models. We compare these to density matrix renormalization group (DMRG) calculations, and find good agreement in the extreme limits. We use these analytical results to interpret the DMRG calculations in the intermediate-coupling regime (defined by W~U), most applicable to conjugated polymers. We make the following conclusions. (1) In the weak-coupling limit the bound states are Mott-Wannier excitons, i.e., conduction-band electrons bound to valence-band holes. Singlet and triplet excitons whose relative wave functions are odd under a reflection of the relative coordinate are degenerate. Thus, the 2 1A+g and 1 3A-g states are degenerate in this limit. (2) In the strong-coupling limit the bound states are Mott-Hubbard excitons, i.e., particles in the upper Hubbard band bound to holes in the lower Hubbard band. These bound states occur in doublets of even and odd parity excitons. Triplet excitons are magnons bound to the singlet excitons, and hence are degenerate with their singlet counterparts. (3) In the intermediate-coupling regime Mott-Wannier excitons are the more appropriate description for large dimerization, while for the undimerized chain Mott-Hubbard excitons are the correct description. For dimerizations relevant to polyacetylene and polydiacetylene both Mott-Hubbard and Mott-Wannier excitons are present. (4) For all coupling strengths an infinite number of bound states exist for 1/r interactions for an infinite polymer. As a result of the discreteness of the lattice and the restrictions on the exciton wave functions in one dimension, the progression of states does not follow the Rydberg series. In practice, excitons whose particle-hole separation exceeds the length of the polymer

  17. Exciton binding energy in a pyramidal quantum dot

    Science.gov (United States)

    Anitha, A.; Arulmozhi, M.

    2018-05-01

    The effects of spatially dependent effective mass, non-parabolicity of the conduction band and dielectric screening function on exciton binding energy in a pyramid-shaped quantum dot of GaAs have been investigated by variational method as a function of base width of the pyramid. We have assumed that the pyramid has a square base with area a× a and height of the pyramid H=a/2. The trial wave function of the exciton has been chosen according to the even mirror boundary condition, i.e. the wave function of the exciton at the boundary could be non-zero. The results show that (i) the non-parabolicity of the conduction band affects the light hole (lh) and heavy hole (hh) excitons to be more bound than that with parabolicity of the conduction band, (ii) the dielectric screening function (DSF) affects the lh and hh excitons to be more bound than that without the DSF and (iii) the spatially dependent effective mass (SDEM) affects the lh and hh excitons to be less bound than that without the SDEM. The combined effects of DSF and SDEM on exciton binding energy have also been calculated. The results are compared with those available in the literature.

  18. Effect of exciton polaritons of absorption edge of GaTe

    International Nuclear Information System (INIS)

    Kurbatov, L.N.; Dirochka, A.I.; Sosin, V.A.

    1979-01-01

    The experimental results, pointing to the dependence of spectral and integral coefficients of exciton absorption as well as to the exciton relaxation parameter γsub(0) over the exciton zone on the sample thickness, are presented. It is tried to explain the inverse dependences of absorption intensity in the maximum of αsub(max) and γsub(0) exciton line within the limits of polariton theory. The values of polariton free path length in GaTe at various temperatures, as well as the volume γsub(vol.) and surface γsub(surf.) parameters of exciton relaxation over the exciton zone are discussed

  19. Numerical modeling of exciton-polariton Bose-Einstein condensate in a microcavity

    Science.gov (United States)

    Voronych, Oksana; Buraczewski, Adam; Matuszewski, Michał; Stobińska, Magdalena

    2017-06-01

    A novel, optimized numerical method of modeling of an exciton-polariton superfluid in a semiconductor microcavity was proposed. Exciton-polaritons are spin-carrying quasiparticles formed from photons strongly coupled to excitons. They possess unique properties, interesting from the point of view of fundamental research as well as numerous potential applications. However, their numerical modeling is challenging due to the structure of nonlinear differential equations describing their evolution. In this paper, we propose to solve the equations with a modified Runge-Kutta method of 4th order, further optimized for efficient computations. The algorithms were implemented in form of C++ programs fitted for parallel environments and utilizing vector instructions. The programs form the EPCGP suite which has been used for theoretical investigation of exciton-polaritons. Catalogue identifier: AFBQ_v1_0 Program summary URL:http://cpc.cs.qub.ac.uk/summaries/AFBQ_v1_0.html Program obtainable from: CPC Program Library, Queen's University, Belfast, N. Ireland Licensing provisions: BSD-3 No. of lines in distributed program, including test data, etc.: 2157 No. of bytes in distributed program, including test data, etc.: 498994 Distribution format: tar.gz Programming language: C++ with OpenMP extensions (main numerical program), Python (helper scripts). Computer: Modern PC (tested on AMD and Intel processors), HP BL2x220. Operating system: Unix/Linux and Windows. Has the code been vectorized or parallelized?: Yes (OpenMP) RAM: 200 MB for single run Classification: 7, 7.7. Nature of problem: An exciton-polariton superfluid is a novel, interesting physical system allowing investigation of high temperature Bose-Einstein condensation of exciton-polaritons-quasiparticles carrying spin. They have brought a lot of attention due to their unique properties and potential applications in polariton-based optoelectronic integrated circuits. This is an out-of-equilibrium quantum system confined

  20. Sagnac interferometry with coherent vortex superposition states in exciton-polariton condensates

    Science.gov (United States)

    Moxley, Frederick Ira; Dowling, Jonathan P.; Dai, Weizhong; Byrnes, Tim

    2016-05-01

    We investigate prospects of using counter-rotating vortex superposition states in nonequilibrium exciton-polariton Bose-Einstein condensates for the purposes of Sagnac interferometry. We first investigate the stability of vortex-antivortex superposition states, and show that they survive at steady state in a variety of configurations. Counter-rotating vortex superpositions are of potential interest to gyroscope and seismometer applications for detecting rotations. Methods of improving the sensitivity are investigated by targeting high momentum states via metastable condensation, and the application of periodic lattices. The sensitivity of the polariton gyroscope is compared to its optical and atomic counterparts. Due to the large interferometer areas in optical systems and small de Broglie wavelengths for atomic BECs, the sensitivity per detected photon is found to be considerably less for the polariton gyroscope than with competing methods. However, polariton gyroscopes have an advantage over atomic BECs in a high signal-to-noise ratio, and have other practical advantages such as room-temperature operation, area independence, and robust design. We estimate that the final sensitivities including signal-to-noise aspects are competitive with existing methods.

  1. Switching Exciton Pulses Through Conical Intersections

    Science.gov (United States)

    Leonhardt, K.; Wüster, S.; Rost, J. M.

    2014-11-01

    Exciton pulses transport excitation and entanglement adiabatically through Rydberg aggregates, assemblies of highly excited light atoms, which are set into directed motion by resonant dipole-dipole interaction. Here, we demonstrate the coherent splitting of such pulses as well as the spatial segregation of electronic excitation and atomic motion. Both mechanisms exploit local nonadiabatic effects at a conical intersection, turning them from a decoherence source into an asset. The intersection provides a sensitive knob controlling the propagation direction and coherence properties of exciton pulses. The fundamental ideas discussed here have general implications for excitons on a dynamic network.

  2. Exciton-relaxation dynamics in lead halides

    International Nuclear Information System (INIS)

    Iwanaga, Masanobu; Hayashi, Tetsusuke

    2003-01-01

    We survey recent comprehensive studies of exciton relaxation in the crystals of lead halides. The luminescence and electron-spin-resonance studies have revealed that excitons in lead bromide spontaneously dissociate and both electrons and holes get self-trapped individually. Similar relaxation has been also clarified in lead chloride. The electron-hole separation is ascribed to repulsive correlation via acoustic phonons. Besides, on the basis of the temperature profiles of self-trapped states, we discuss the origin of luminescence components which are mainly induced under one-photon excitation into the exciton band in lead fluoride, lead chloride, and lead bromide

  3. Excitonic effects in the luminescence of quantum wells

    International Nuclear Information System (INIS)

    Deveaud, B.; Kappei, L.; Berney, J.; Morier-Genoud, F.; Portella-Oberli, M.T.; Szczytko, J.; Piermarocchi, C.

    2005-01-01

    We report on the origin of the excitonic luminescence in quantum wells. This study is carried out by time-resolved photoluminescence experiments performed on a very high-quality InGaAs quantum well sample in which the photoluminescence contributions at the energy of the exciton and at the band edge can be clearly separated and traced over a broad range of times and densities. This allows us to compare the two conflicting theoretical approaches to the question of the origin of the excitonic luminescence in quantum wells: the model of the exciton population and the model of the Coulomb correlated plasma. We measure the exciton formation time and we show the fast exciton formation and its dependence with carrier density. We are also able to give the boundaries of the Mott transition in our system, and to show the absence of observable renormalization of the gap below the onset of this transition. We detail the characteristics of the trion formation and evidence the possible formation of both positive and negative trions in the absence of any resident free carrier populations

  4. Excitons in van der Waals heterostructures

    DEFF Research Database (Denmark)

    Latini, Simone; Olsen, Thomas; Thygesen, Kristian Sommer

    2015-01-01

    The existence of strongly bound excitons is one of the hallmarks of the newly discovered atomically thin semiconductors. While it is understood that the large binding energy is mainly due to the weak dielectric screening in two dimensions, a systematic investigation of the role of screening on two......-dimensional (2D) excitons is still lacking. Here we provide a critical assessment of a widely used 2D hydrogenic exciton model, which assumes a dielectric function of the form epsilon(q) = 1 + 2 pi alpha q, and we develop a quasi-2D model with a much broader applicability. Within the quasi-2D picture, electrons...... exciton binding energies in both isolated and supported 2D materials. For isolated 2D materials, the quasi-2D treatment yields results almost identical to those of the strict 2D model, and both are in good agreement with ab initio many-body calculations. On the other hand, for more complex structures...

  5. Exciton-phonon coupling in a CsPbBr3 single nanocrystal

    Science.gov (United States)

    Ramade, Julien; Andriambariarijaona, Léon Marcel; Steinmetz, Violette; Goubet, Nicolas; Legrand, Laurent; Barisien, Thierry; Bernardot, Frédérick; Testelin, Christophe; Lhuillier, Emmanuel; Bramati, Alberto; Chamarro, Maria

    2018-02-01

    We have performed micro-photoluminescence measurements on a single CsPbBr3 nanocrystal (NC) with a size comparable to the Bohr diameter (7 nm). When the NC has an orthorhombic crystal symmetry, we observe an exciton fine structure composed of three peaks linearly polarized. We took advantage of the polarization properties of micro-photoluminescence to monitor in situ both the energy and linewidth of individual peaks when increasing temperature. We reveal that two regimes exist, at low and high temperature, which are dominated by acoustic or longitudinal optical phonon (Fröhlich term) couplings, respectively. The acoustic contribution does not change when the energy of the excitonic transition varies in the range of 2.46-2.62 eV, i.e., with NC sizes corresponding to this range. We find that line broadening is mainly ruled by the Fröhlich term, which is consistent with the polar nature of CsPbBr3.

  6. Synthesis and Exciton Dynamics of Triplet Sensitized Conjugated Polymers

    KAUST Repository

    Andernach, Rolf

    2015-07-22

    We report the synthesis of a novel polythiophene-based host-guest copolymer incorporating a Pt-porphyrin complex (TTP-Pt) into the backbone for efficient singlet to triplet polymer exciton sensitization. We elucidated the exciton dynamics in thin films of the material by means of Transient Absorption Spectrosopcy (TAS) on multiple timescales and investigated the mechanism of triplet exciton formation. During sensitization, single exciton diffusion is followed by exciton transfer from the polymer backbone to the complex where it undergoes intersystem crossing to the triplet state of the complex. We directly monitored the triplet exciton back transfer from the Pt-porphyrin to the polymer and find that 60% of the complex triplet excitons are transferred with a time constant of 1087 ps. We propose an equilibrium between polymer and porphyrin triplet states as a result of the low triplet diffusion length in the polymer backbone and hence an increased local triplet population resulting in increased triplet-triplet annihilation. This novel system has significant implications for the design of novel materials for triplet sensitized solar cells and up-conversion layers.

  7. Excitonic polaritons of zinc diarsenide single crystals

    Energy Technology Data Exchange (ETDEWEB)

    Syrbu, N.N., E-mail: sirbunn@yahoo.com [Technical University of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of); Stamov, I.G. [T.G. Shevchenko State University of Pridnestrovie, Tiraspol, Republic of Moldova (Moldova, Republic of); Zalamai, V.V. [Institute of Applied Physics, Academy of Sciences of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of); Dorogan, A. [Technical University of Moldova, Chisinau, Republic of Moldova (Moldova, Republic of)

    2017-02-01

    Excitonic polaritons of ZnAs{sub 2} single crystals had been investigated. Parameters of singlet excitons with Г{sub 2}¯(z) symmetry and orthoexcitons 2Г{sub 1}¯(y)+Г{sub 2}¯(x) had been determined. Spectral dependencies of ordinary and extraordinary dispersion of refractive index had been calculated using interferential reflection and transmittance spectra. It was shown, that A excitonic series were due to hole (V{sub 1}) and electron (C{sub 1}) bands. The values of effective masses of electrons (m{sub c}{sup *}=0.10 m{sub 0}) and holes (m{sub v1}{sup *}=0.89 m{sub 0}) had been estimated. It was revealed that the hole mass m{sub v1}{sup *} changes from 1.03 m{sub 0} to 0.55 m{sub 0} at temperature increasing from 10 K up to 230 K and that the electron mass m{sub c}{sup *} does not depend on temperature. The integral absorption A (eV cm{sup −1}) of the states n=1, 2 and 3 of Г{sub 2}¯(z) excitons depends on the A{sub n}≈n{sup −3} equality, which it is characteristic for S-type excitonic functions. Temperature dependences of the integral absorption of ground states for Г{sub 2}¯(z) and Г{sub 2}¯(Ñ…) excitons differ. The ground states of B and C excitons formed by V{sub 3} – C{sub 1} and V{sub 4} – C{sub 1} bands and its parameters had been determined.

  8. Oxygen Passivation Mediated Tunability of Trion and Excitons in MoS2

    KAUST Repository

    Gogoi, Pranjal Kumar

    2017-08-17

    Using wide spectral range in situ spectroscopic ellipsometry with systematic ultrahigh vacuum annealing and in situ exposure to oxygen, we report the complex dielectric function of MoS2 isolating the environmental effects and revealing the crucial role of unpassivated and passivated sulphur vacancies. The spectral weights of the A (1.92 eV) and B (2.02 eV) exciton peaks in the dielectric function reduce significantly upon annealing, accompanied by spectral weight transfer in a broad energy range. Interestingly, the original spectral weights are recovered upon controlled oxygen exposure. This tunability of the excitonic effects is likely due to passivation and reemergence of the gap states in the band structure during oxygen adsorption and desorption, respectively, as indicated by ab initio density functional theory calculation results. This Letter unravels and emphasizes the important role of adsorbed oxygen in the optical spectra and many-body interactions of MoS2.

  9. Coherence properties of exciton polariton OPO condensates in one and two dimensions

    International Nuclear Information System (INIS)

    Spano, R; Cuadra, J; Tosi, G; Antón, C; Lingg, C A; Sanvitto, D; Martín, M D; Viña, L; Eastham, P R; Van der Poel, M; Hvam, J M

    2012-01-01

    We give an overview of the coherence properties of exciton-polariton condensates generated by optical parametric scattering. Different aspects of the first-order coherence (g (1) ) have been investigated. The spatial coherence extension of a two-dimensional (2D) polariton system, below and at the parametric threshold, demonstrates the development of a constant phase coherence over the entire condensate, once the condensate phase transition takes place. The effect on coherence of the photonic versus excitonic nature of the condensates is also examined. The coherence of a quasi-1D trap, composed of a line defect, is studied, showing the detrimental effect of reduced dimensionality on the establishment of the long range order. In addition, the temporal coherence decay, g (1) (τ), reveals a fast decay in contrast with the 2D case. The situation of a quasi-1D condensate coexisting with a 2D one is also presented. (paper)

  10. Oxygen Passivation Mediated Tunability of Trion and Excitons in MoS2

    Science.gov (United States)

    Gogoi, Pranjal Kumar; Hu, Zhenliang; Wang, Qixing; Carvalho, Alexandra; Schmidt, Daniel; Yin, Xinmao; Chang, Yung-Huang; Li, Lain-Jong; Sow, Chorng Haur; Neto, A. H. Castro; Breese, Mark B. H.; Rusydi, Andrivo; Wee, Andrew T. S.

    2017-08-01

    Using wide spectral range in situ spectroscopic ellipsometry with systematic ultrahigh vacuum annealing and in situ exposure to oxygen, we report the complex dielectric function of MoS2 isolating the environmental effects and revealing the crucial role of unpassivated and passivated sulphur vacancies. The spectral weights of the A (1.92 eV) and B (2.02 eV) exciton peaks in the dielectric function reduce significantly upon annealing, accompanied by spectral weight transfer in a broad energy range. Interestingly, the original spectral weights are recovered upon controlled oxygen exposure. This tunability of the excitonic effects is likely due to passivation and reemergence of the gap states in the band structure during oxygen adsorption and desorption, respectively, as indicated by ab initio density functional theory calculation results. This Letter unravels and emphasizes the important role of adsorbed oxygen in the optical spectra and many-body interactions of MoS2 .

  11. Oxygen Passivation Mediated Tunability of Trion and Excitons in MoS2

    KAUST Repository

    Gogoi, Pranjal Kumar; Hu, Zhenliang; Wang, Qixing; Carvalho, Alexandra; Schmidt, Daniel; Yin, Xinmao; Chang, Yung-Huang; Li, Lain-Jong; Sow, Chorng Haur; Neto, A.  H. Castro; Breese, Mark B.  H.; Rusydi, Andrivo; Wee, Andrew T.  S.

    2017-01-01

    Using wide spectral range in situ spectroscopic ellipsometry with systematic ultrahigh vacuum annealing and in situ exposure to oxygen, we report the complex dielectric function of MoS2 isolating the environmental effects and revealing the crucial role of unpassivated and passivated sulphur vacancies. The spectral weights of the A (1.92 eV) and B (2.02 eV) exciton peaks in the dielectric function reduce significantly upon annealing, accompanied by spectral weight transfer in a broad energy range. Interestingly, the original spectral weights are recovered upon controlled oxygen exposure. This tunability of the excitonic effects is likely due to passivation and reemergence of the gap states in the band structure during oxygen adsorption and desorption, respectively, as indicated by ab initio density functional theory calculation results. This Letter unravels and emphasizes the important role of adsorbed oxygen in the optical spectra and many-body interactions of MoS2.

  12. Robust adiabatic approach to optical spin entangling in coupled quantum dots

    International Nuclear Information System (INIS)

    Gauger, Erik M; Benjamin, Simon C; Lovett, Brendon W; Nazir, Ahsan; Stace, Thomas M

    2008-01-01

    Excitonic transitions offer a possible route to ultrafast optical spin manipulation in coupled nanostructures. We perform here a detailed study of the three principal exciton-mediated decoherence channels for optically controlled electron spin qubits in coupled quantum dots: radiative decay of the excitonic state, exciton-phonon interactions, and Landau-Zener transitions between laser-dressed states. We consider a scheme for producing an entangling controlled-phase gate on a pair of coupled spins which, in its simplest dynamic form, renders the system subject to fast decoherence rates associated with exciton creation during the gating operation. In contrast, we show that an adiabatic approach employing off-resonant laser excitation allows us to suppress all sources of decoherence simultaneously, significantly increasing the fidelity of operations at only a relatively small gating time cost. We find that controlled-phase gates accurate to one part in 10 2 can realistically be achieved with the adiabatic approach, whereas the conventional dynamic approach does not appear to support a fidelity suitable for scalable quantum computation. Our predictions could be demonstrated experimentally in the near future

  13. Quantum theory of the optical and electronic properties of semiconductors

    CERN Document Server

    Haug, Hartmut

    2009-01-01

    This invaluable textbook presents the basic elements needed to understand and research into semiconductor physics. It deals with elementary excitations in bulk and low-dimensional semiconductors, including quantum wells, quantum wires and quantum dots. The basic principles underlying optical nonlinearities are developed, including excitonic and many-body plasma effects. Fundamentals of optical bistability, semiconductor lasers, femtosecond excitation, the optical Stark effect, the semiconductor photon echo, magneto-optic effects, as well as bulk and quantum-confined Franz-Keldysh effects, are covered. The material is presented in sufficient detail for graduate students and researchers with a general background in quantum mechanics.This fifth edition includes an additional chapter on 'Quantum Optical Effects' where the theory of quantum optical effects in semiconductors is detailed. Besides deriving the 'semiconductor luminescence equations' and the expression for the stationary luminescence spectrum, the resu...

  14. Optical absorption and energy transport in compact dendrimers with unsymmetrical branching

    International Nuclear Information System (INIS)

    Supritz, C.; Gounaris, V.; Reineker, P.

    2008-01-01

    We investigate the linear optical absorption and the energy transport in compact dendrimers with unsymmetrical branching, using the Frenkel exciton concept. The electron-phonon interaction is taken into account by introducing a heat bath that interacts with the exciton in a stochastic manner

  15. Two-photon transitions to exciton polaritons

    International Nuclear Information System (INIS)

    Hassan, A.R.

    1979-08-01

    A semiclassical theory for the creation of excitonic polariton states by two-photon absorption, via an intermediate exciton state, is given. A band model has been introduced which gives the dominant contribution to this process. A numerical calculation is found to be in good agreement with a recent observation in CuCl. (author)

  16. Excitons in InP/InAs inhomogeneous quantum dots

    International Nuclear Information System (INIS)

    Assaid, E; Feddi, E; Khamkhami, J El; Dujardin, F

    2003-01-01

    Wannier excitons confined in an InP/InAs inhomogeneous quantum dot (IQD) have been studied theoretically in the framework of the effective mass approximation. A finite-depth potential well has been used to describe the effect of the quantum confinement in the InAs layer. The exciton binding energy has been determined using the Ritz variational method. The spatial correlation between the electron and the hole has been taken into account in the expression for the wavefunction. It has been shown that for a fixed size b of the IQD, the exciton binding energy depends strongly on the core radius a. Moreover, it became apparent that there are two critical values of the core radius, a crit and a 2D , for which important changes of the exciton binding occur. The former critical value, a crit , corresponds to a minimum of the exciton binding energy and may be used to distinguish between tridimensional confinement and bidimensional confinement. The latter critical value, a 2D , corresponds to a maximum of the exciton binding energy and to the most pronounced bidimensional character of the exciton

  17. Exciton polariton spectra and limiting factors for the room-temperature photoluminescence efficiency in ZnO

    Science.gov (United States)

    Chichibu, S. F.; Uedono, A.; Tsukazaki, A.; Onuma, T.; Zamfirescu, M.; Ohtomo, A.; Kavokin, A.; Cantwell, G.; Litton, C. W.; Sota, T.; Kawasaki, M.

    2005-04-01

    Static and dynamic responses of excitons in state-of-the-art bulk and epitaxial ZnO are reviewed to support the possible realization of polariton lasers, which are coherent and monochromatic light sources due to Bose condensation of exciton-polaritons in semiconductor microcavities (MCs). To grasp the current problems and to pave the way for obtaining ZnO epilayers of improved quality, the following four principal subjects are treated: (i) polarized optical reflectance (OR), photoreflectance (PR) and photoluminescence (PL) spectra of the bulk and epitaxial ZnO were recorded at 8 K. Energies of PR resonances corresponded to those of upper and lower exciton-polariton branches, where A-, B- and C-excitons couple simultaneously to an electromagnetic wave. PL peaks due to the corresponding polariton branches were observed. Longitudinal-transverse splittings (ωLT) of the corresponding excitons were 1.5, 11.1 and 13.1 meV, respectively. The latter two values are more than two orders of magnitude greater than that of GaAs being 0.08 meV. (ii) Using these values and material parameters, corresponding vacuum-field Rabi splitting of exciton-polaritons coupled to a model MC mode was calculated to be 191 meV, which is the highest value ever reported for semiconductor MCs and satisfies the requirements to observe the strong exciton-light coupling regime necessary for polariton lasing above room temperature. (iii) Polarized OR and PR spectra of an out-plane nonpolar (1\\,1\\,\\bar{2}\\,0) ZnO epilayer grown by laser-assisted molecular beam epitaxy (L-MBE) were measured, since ZnO quantum wells (QWs) grown in nonpolar orientations are expected to show higher emission efficiencies due to the elimination of spontaneous and piezoelectric polarization fields normal to the QW plane. They exhibited in-plane anisotropic exciton resonances according to the polarization selection rules for anisotropically-strained wurzite material. (iv) Impacts of point defects on the nonradiative

  18. Numerical study on electronic and optical properties of organic light emitting diodes.

    Science.gov (United States)

    Kim, Kwangsik; Hwang, Youngwook; Won, Taeyoung

    2013-08-01

    In this paper, we present a finite element method (FEM) study of space charge effects in organic light emitting diodes. Our model includes a Gaussian density of states to account for the energetic disorder in organic semiconductors and the Fermi-Dirac statistics to account for the charge hopping process between uncorrelated sites. The physical model cover all the key physical processes in OLEDs, namely charge injection, transport and recombination, exciton diffusion, transfer and decay as well as light coupling, and thin-film-optics. The exciton model includes generation, diffusion, and energy transfer as well as annihilation. We assumed that the light emission originates from oscillating and thus embodied as excitons and embedded in a stack of multilayer. The out-coupled emission spectrum has been numerically calculated as a function of viewing angle, polarization, and dipole orientation. We discuss the accumulation of charges at internal interfaces and their signature in the transient response as well as the electric field distribution.

  19. Exciton spectra of mixed LiH1-xDx crystals

    International Nuclear Information System (INIS)

    Plekhanov, V.G.

    1989-01-01

    The results of low-tempertaure experimental investigation of exciton spectra of pure surface of mixed crystals LiH 1-x d x forming the continuous series of a solved solution are presented. The long-wave reflection spectra is formed, as in pure crystals, by excitons of a large radius. The developed structure of spectra of exciton luminiscence consisting mainly of LO-lines, testifies to the intraband Frelich mechanism of free exciton scattering by LO-phonos, playing the considerable role in renormalization of the exciton Rydberg and the energy of interband transitions. Increase of the concentration of deuterium in mixed crystals causes a short-wave shift in the reflection spectrum and luminescence and continuous decrease of LO-phonon energy together with the increase of Rydberg exciton

  20. New method for control over exciton states in quantum wells

    International Nuclear Information System (INIS)

    Maslov, A Yu; Proshina, O V

    2010-01-01

    The theoretical study of the exciton states in the quantum well is performed with regard to the distinctions of the dielectric properties of quantum well and barrier materials. The strong exciton-phonon interaction is shown to be possible in materials with high ionicity. This leads to the essential modification of the exciton states. The relationship between the exciton binding energy, along with oscillator strength and the barrier material dielectric properties is found. This suggests the feasibility of the exciton spectrum parameter control by the choice of the barrier material. It is shown that such exciton spectrum engineering also is possible in the quantum wells based on the materials with low ionicity. The reason is the dielectric confinement effect in the quantum wells.

  1. Femtosecond dynamics of excitons in π-conjugated oligomers: the role of intrachain two-exciton states in the formation of interchain species

    Science.gov (United States)

    Klimov, Victor I.; McBranch, Duncan W.; Barashkov, Nikolay N.; Ferraris, John P.

    1997-10-01

    We report femtosecond transient absorption results for solutions and thin films of a substituted oligomer of poly(para-phenylene vinylene) performed over wide spectral and pump-intensity ranges. Solutions and films exhibit a photoinduced absorption (PA) band with dynamics matching those of the stimulated emission, demonstrating unambiguously that these features originate from intrachain singlet excitons. Thin films exhibit an additional short-wavelength PA band with pump-independent dynamics, indicating the formation of non-emissive interchain excitons. Correlations in the dynamics of the two PA features, as well as the intensity-dependence, provide strong evidence that the formation of interchain excitons is mediated by intrachain two-exciton states.

  2. Optical gain for the interband optical transition in InAsP/InP quantum well wire in the influence of laser field intensity

    Energy Technology Data Exchange (ETDEWEB)

    Saravanan, S. [Dept.of Physics, GTN Arts College, Dindigul-624 005. India (India); Peter, A. John, E-mail: a.john.peter@gmail.com [P.G & Research Dept.of Physics, Government Arts College, Melur-625 106. Madurai. India (India)

    2016-05-23

    Intense high frequency laser field induced electronic and optical properties of heavy hole exciton in the InAs{sub 0.8}P{sub 0.2}/InP quantum wire is studied taking into account the geometrical confinement effect. Laser field related exciton binding energies and the optical band gap in the InAs{sub 0.8}P{sub 0.2}/InP quantum well wire are investigated. The optical gain, for the interband optical transition, as a function of photon energy, in the InAs{sub 0.8}P{sub 0.2}/InP quantum wire, is obtained in the presence of intense laser field. The compact density matrix method is employed to obtain the optical gain. The obtained optical gain in group III-V narrow quantum wire can be applied for achieving the preferred telecommunication wavelength.

  3. Triplet exciton formation in organic photovoltaics

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Xudong; Westenhoff, Sebastian; Howard, Ian; Ford, Thomas; Friend, Richard; Hodgkiss, Justin; Greenham, Neil [Cavendish Laboratory, University of Cambridge (United Kingdom)

    2009-07-01

    We have recently found that the formation of triplet excitons can be an important loss mechanism in organic photovoltaics, particularly in donor-acceptor blends designed to have high open-circuit voltages. This can occur when the intrachain triplet state lies lower in energy than the charge-transfer state formed at the heterojunction. We find that in a blend based on the polyfluorene derivatives F8BT and PFB, triplet excitons are formed after photoexcitation with much higher efficiency than in the component polymers. We use transient absorption spectroscopy to study the dynamics of charges and triplet excitons on timescales from picoseconds to microseconds. This allows us to determine a characteristic time of {proportional_to} 40 ns for intersystem crossing in the charge-separated state, and to estimate that as many as 75% of photoexcitations lead to the formation of triplet states. To avoid losses to triplet excitons in photovoltaic devices, it is necessary to separate charge pairs before intersystem crossing can occur. We also present photophysical measurements of saturation and relaxation of the triplet excited state absorption used to quantify triplet populations.

  4. Semiconductor Optics

    CERN Document Server

    Klingshirn, Claus F

    2012-01-01

    This updated and enlarged new edition of Semiconductor Optics provides an introduction to and an overview of semiconductor optics from the IR through the visible to the UV, including linear and nonlinear optical properties, dynamics, magneto and electrooptics, high-excitation effects and laser processes, some applications, experimental techniques and group theory. The mathematics is kept as elementary as possible, sufficient for an intuitive understanding of the experimental results and techniques treated. The subjects covered extend from physics to materials science and optoelectronics. Significantly updated chapters add coverage of current topics such as electron hole plasma, Bose condensation of excitons and meta materials. Over 120 problems, chapter introductions and a detailed index make it the key textbook for graduate students in physics. The mathematics is kept as elementary as possible, sufficient for an intuitive understanding of the experimental results and techniques treated. The subjects covered ...

  5. Exciton ionization in multilayer transition-metal dichalcogenides

    DEFF Research Database (Denmark)

    Pedersen, Thomas Garm; Latini, Simone; Thygesen, Kristian Sommer

    2016-01-01

    Photodetectors and solar cells based on materials with strongly bound excitons rely crucially on field-assisted exciton ionization. We study the ionization process in multilayer transition-metal dichalcogenides (TMDs) within the Mott-Wannier model incorporating fully the pronounced anisotropy...

  6. Optical orientation of the homogeneous nonequilibrium Bose-Einstein condensate of exciton polaritons

    Science.gov (United States)

    Korenev, V. L.

    2012-07-01

    A simple model, describing the steady state of the nonequilibrium polarization of a homogeneous Bose-Einstein condensate of exciton polaritons, is considered. It explains the suppression of spin splitting of a nonequilibrium polariton condensate in an external magnetic field, the linear polarization, the linear-to-circular polarization conversion, and the unexpected sign of the circular polarization of the condensate all on equal footing. It is shown that inverse effects are possible, to wit, spontaneous circular polarization and the enhancement of spin splitting of a nonequilibrium condensate of polaritons.

  7. Ab initio calculation of the electronic and optical properties of solid pentacene

    International Nuclear Information System (INIS)

    Tiago, Murilo L.; Northrup, John E.; Louie, Steve G.

    2002-01-01

    The optical and electronic properties of crystalline pentacene are studied, using a first-principles Green's-function approach. The quasiparticle energies are calculated within the GW approximation and the electron-hole excitations are computed by solving the Bethe-Salpeter equation. We investigate the role of polymorphism on the electronic energy gap and linear optical spectrum by studying two different crystalline phases: the solution-phase structure and the vapor-phase structure. charge-transfer excitons are found to dominate the optical spectrum. Excitons with sizable binding energies are predicted for both phases

  8. Relaxation of nonthermal hh and lh excitons in ZnSe quantum wells

    DEFF Research Database (Denmark)

    Kalt, H.; Hoffmann, J.; Umlauff, M.

    1998-01-01

    The strong exciton-LO phonon coupling in ZnSe QWs gives a direct access to the relaxation dynamics of nonthermal, free heavy-hole and light-hole excitons. Narrow hot-exciton distributions can be generated by LO-phonon assisted exciton formation. The thermalization of these excitons is monitored b...

  9. Organic photovoltaic cell incorporating electron conducting exciton blocking layers

    Science.gov (United States)

    Forrest, Stephen R.; Lassiter, Brian E.

    2014-08-26

    The present disclosure relates to photosensitive optoelectronic devices including a compound blocking layer located between an acceptor material and a cathode, the compound blocking layer including: at least one electron conducting material, and at least one wide-gap electron conducting exciton blocking layer. For example, 3,4,9,10 perylenetetracarboxylic bisbenzimidazole (PTCBI) and 1,4,5,8-napthalene-tetracarboxylic-dianhydride (NTCDA) function as electron conducting and exciton blocking layers when interposed between the acceptor layer and cathode. Both materials serve as efficient electron conductors, leading to a fill factor as high as 0.70. By using an NTCDA/PTCBI compound blocking layer structure increased power conversion efficiency is achieved, compared to an analogous device using a conventional blocking layers shown to conduct electrons via damage-induced midgap states.

  10. Excitonic polarons in quasi-one-dimensional LH1 and LH2 bacteriochlorophyll a antenna aggregates from photosynthetic bacteria: A wavelength-dependent selective spectroscopy study

    International Nuclear Information System (INIS)

    Freiberg, Arvi; Raetsep, Margus; Timpmann, Kou; Trinkunas, Gediminas

    2009-01-01

    Spectral characteristics of the optically excited states in the ring-shaped quasi-one-dimensional aggregates comprising 18 and 32 tightly coupled bacteriochlorophyll a molecules have been investigated using selective spectroscopy methods and theoretical modelling of the data. Distinguished by the lowest electronic transition energies in the LH2 and LH1 antenna complexes these aggregates govern the functionally important ultrafast funneling of solar excitation energy in the photosynthetic membranes of purple bacteria. It was found by using a sophisticated differential fluorescence line narrowing method that exciton-phonon coupling in terms of the dimensionless Huang-Rhys factor is strong in these systems, justifying an excitonic polaron theoretical approach for the data analysis. Although we reached this qualitative conclusion already previously, in this work essential dependence of the exciton-phonon coupling strength and reorganization energy on excitation wavelength as well as on excitation light fluence has been established. We then show that these results corroborate with the properties of excitonic polarons in diagonally disordered ensembles of the aggregates. Furthermore, the weighted density of states of the phonon modes, which is an important characteristic of dynamical systems interacting with their surroundings, was derived. Its shape, being similar for all studied circular aggregates, deviates significantly from a reference profile describing local response of a protein to the Q y electronic transition in a single bacteriochlorophyll a molecule. Similarities of the data for regular and B800 deficient mutant LH2 complexes indicate that the B800 pigments have no direct influence on the electronic states of the B850 aggregate system. Consistent set of model parameters was determined, unambiguously implying that excitonic polarons, rather than bare excitons are proper lowest-energy optical excitations in the LH1 and LH2 antenna complexes

  11. Excitonic polarons in quasi-one-dimensional LH1 and LH2 bacteriochlorophyll a antenna aggregates from photosynthetic bacteria: A wavelength-dependent selective spectroscopy study

    Energy Technology Data Exchange (ETDEWEB)

    Freiberg, Arvi [Institute of Physics, University of Tartu, Riia 142, 51014 Tartu (Estonia); Institute of Molecular and Cell Biology, University of Tartu, Riia 23, 51010 Tartu (Estonia)], E-mail: arvi.freiberg@ut.ee; Raetsep, Margus; Timpmann, Kou [Institute of Physics, University of Tartu, Riia 142, 51014 Tartu (Estonia); Trinkunas, Gediminas [Insitute of Physics, Savanoriu pr. 231, LT-02300 Vilnius (Lithuania)

    2009-02-23

    Spectral characteristics of the optically excited states in the ring-shaped quasi-one-dimensional aggregates comprising 18 and 32 tightly coupled bacteriochlorophyll a molecules have been investigated using selective spectroscopy methods and theoretical modelling of the data. Distinguished by the lowest electronic transition energies in the LH2 and LH1 antenna complexes these aggregates govern the functionally important ultrafast funneling of solar excitation energy in the photosynthetic membranes of purple bacteria. It was found by using a sophisticated differential fluorescence line narrowing method that exciton-phonon coupling in terms of the dimensionless Huang-Rhys factor is strong in these systems, justifying an excitonic polaron theoretical approach for the data analysis. Although we reached this qualitative conclusion already previously, in this work essential dependence of the exciton-phonon coupling strength and reorganization energy on excitation wavelength as well as on excitation light fluence has been established. We then show that these results corroborate with the properties of excitonic polarons in diagonally disordered ensembles of the aggregates. Furthermore, the weighted density of states of the phonon modes, which is an important characteristic of dynamical systems interacting with their surroundings, was derived. Its shape, being similar for all studied circular aggregates, deviates significantly from a reference profile describing local response of a protein to the Q{sub y} electronic transition in a single bacteriochlorophyll a molecule. Similarities of the data for regular and B800 deficient mutant LH2 complexes indicate that the B800 pigments have no direct influence on the electronic states of the B850 aggregate system. Consistent set of model parameters was determined, unambiguously implying that excitonic polarons, rather than bare excitons are proper lowest-energy optical excitations in the LH1 and LH2 antenna complexes.

  12. Temperature dependent optical properties of ZnO thin film using ellipsometry and photoluminescence

    Science.gov (United States)

    Bouzourâa, M.-B.; Battie, Y.; Dalmasso, S.; Zaïbi, M.-A.; Oueslati, M.; En Naciri, A.

    2018-05-01

    We report the temperature dependence of the dielectric function, the exciton binding energy and the electronic transitions of crystallized ZnO thin film using spectroscopic ellipsometry (SE) and photoluminescence (PL). ZnO layers were prepared by sol-gel method and deposited on crystalline silicon (Si) by spin coating technique. The ZnO optical properties were determined between 300 K and 620 K. Rigorous study of optical responses was achieved in order to demonstrate the quenching exciton of ZnO as a function of temperature. Numerical technique named constrained cubic splines approximation (CCS), Tauc-Lorentz (TL) and Tanguy dispersion models were selected for the ellipsometry data modeling in order to obtain the dielectric function of ZnO. The results reveals that the exciton bound becomes widely flattening at 470 K on the one hand, and on the other that the Tanguy dispersion law is more appropriate for determining the optical responses of ZnO thin film in the temperature range of 300 K-420 K. The Tauc-Lorentz, for its part, reproduces correctly the ZnO dielectric function in 470 K-620 K temperature range. The temperature dependence of the electronic transition given by SE and PL shows that the exciton quenching was observed in 420 K-∼520 K temperature range. This quenching effect can be explained by the equilibrium between the Coulomb force of exciton and its kinetic energy in the film. The kinetic energy was found to induce three degrees of freedom of the exciton.

  13. Conformation-related exciton localization and charge-pair formation in polythiophenes: ensemble and single-molecule study.

    Science.gov (United States)

    Sugimoto, Toshikazu; Habuchi, Satoshi; Ogino, Kenji; Vacha, Martin

    2009-09-10

    We study conformation-dependent photophysical properties of polythiophene (PT) by molecular dynamics simulations and by ensemble and single-molecule optical experiments. We use a graft copolymer consisting of a polythiophene backbone and long polystyrene branches and compare its properties with those obtained on the same polythiophene derivative without the side chains. Coarse-grain molecular dynamics simulations show that in a poor solvent, the PT without the side chains (PT-R) forms a globulelike conformation in which distances between any two conjugated segments on the chain are within the Forster radius for efficient energy transfer. In the PT with the polystyrene branches (PT-PS), the polymer main PT chain retains an extended coillike conformation, even in a poor solvent, and the calculated distances between conjugated segments favor energy transfer only between a few neighboring chromophores. The theoretical predictions are confirmed by measurements of fluorescence anisotropy and fluorescence blinking of the polymers' single chains. High anisotropy ratios and two-state blinking in PT-R are due to localization of the exciton on a single conjugated segment. These signatures of exciton localization are absent in single chains of PT-PS. Electric-field-induced quenching measured as a function of concentration of PT dispersed in an inert matrix showed that in well-isolated chains of PT-PS, the exciton dissociation is an intrachain process and that aggregation of the PT-R chains causes an increase in quenching due to the onset of interchain interactions. Measurements of the field-induced quenching on single chains indicate that in PT-R, the exciton dissociation is a slower process that takes place only after the exciton is localized on one conjugated segment.

  14. Twisted molecular excitons as mediators for changing the angular momentum of light

    Science.gov (United States)

    Zang, Xiaoning; Lusk, Mark T.

    2017-07-01

    Molecules with CN or CN h symmetry can absorb quanta of optical angular momentum to generate twisted excitons with well-defined quasiangular momenta of their own. Angular momentum is conserved in such interactions at the level of a paraxial approximation for the light beam. A sequence of absorption events can thus be used to create a range of excitonic angular momenta. Subsequent decay can produce radiation with a single angular momentum equal to that accumulated. Such molecules can thus be viewed as mediators for changing the angular momentum of light. This sidesteps the need to exploit nonlinear light-matter interactions based on higher-order susceptibilities. A tight-binding paradigm is used to verify angular momentum conservation and demonstrate how it can be exploited to change the angular momentum of light. The approach is then extended to a time-dependent density functional theory setting where the key results are shown to hold in a many-body, multilevel setting.

  15. EDITORIAL: Optical orientation Optical orientation

    Science.gov (United States)

    SAME ADDRESS *, Yuri; Landwehr, Gottfried

    2008-11-01

    priority of the discovery in the literature, which was partly caused by the existence of the Iron Curtain. I had already enjoyed contact with Boris in the 1980s when the two volumes of Landau Level Spectroscopy were being prepared [2]. He was one of the pioneers of magneto-optics in semiconductors. In the 1950s the band structure of germanium and silicon was investigated by magneto-optical methods, mainly in the United States. No excitonic effects were observed and the band structure parameters were determined without taking account of excitons. However, working with cuprous oxide, which is a direct semiconductor with a relative large energy gap, Zakharchenya and his co-worker Seysan showed that in order to obtain correct band structure parameters, it is necessary to take excitons into account [3]. About 1970 Boris started work on optical orientation. Early work by Hanle in Germany in the 1920s on the depolarization of luminescence in mercury vapour by a transverse magnetic field was not appreciated for a long time. Only in the late 1940s did Kastler and co-workers in Paris begin a systematic study of optical pumping, which led to the award of a Nobel prize. The ideas of optical pumping were first applied by Georges Lampel to solid state physics in 1968. He demonstrated optical orientation of free carriers in silicon. The detection method was nuclear magnetic resonance; optically oriented free electrons dynamically polarized the 29Si nuclei of the host lattice. The first optical detection of spin orientation was demonstrated by with the III-V semiconductor GaSb by Parsons. Due to the various interaction mechanisms of spins with their environment, the effects occurring in semiconductors are naturally more complex than those in atoms. Optical detection is now the preferred method to detect spin alignment in semiconductors. The orientation of spins in crystals pumped with circularly polarized light is deduced from the degree of circular polarization of the recombination

  16. Enhancement of exciton radiative recombination for In-doped ZnO nanowires with aluminum cylindrical micropillars

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Jen-Cheng; Liang, Yu-Ting; Cheng, Fang-Ching; Fang, Chia-Hui; Chen, Hung-Ing; Tsai, Chung-Yuan [Graduate Institute of Electro-Optical Engineering and Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Tao-Yuan 333, Taiwan, ROC (China); Jiang, Joe-Air [Department of Bio-Industrial Mechatronics Engineering, National Taiwan University, Taipei 106, Taiwan, ROC (China); Nee, Tzer-En, E-mail: neete@mail.cgu.edu.tw [Graduate Institute of Electro-Optical Engineering and Department of Electronic Engineering, Chang Gung University, 259 Wen-Hwa 1st Road, Kwei-Shan, Tao-Yuan 333, Taiwan, ROC (China)

    2013-04-15

    Zinc oxide (ZnO) has attracted intensive research effort in recent years, due to its unique properties and versatile applications. Recent work on the conservation of surface plasmon (SP) and light through period metal arrays has elucidated the propagation of SP resonance behavior. In this paper, we discuss the enhancement of exciton radiative recombination of the ZnO nanowires with Al cylindrical micropillars. Optical characterization of exciton interacted with SP resonance for indium-doped ZnO nanowires with Al cylindrical micropillars has been also investigated. From photoluminescence spectra of In-doped ZnO nanowires, it is found that the In-doped ZnO nanowires have a blue emission at 425 nm, which resulted from the ZnO band-to-band transition. Prior to the arrays of samples were annealed, a broad green emission centered at 500 nm was observed, which is attributed to ZnO native point defects. The relatively strong green band emission results from the radiative recombination that arises from the ionized oxygen vacancy and surface-defect related luminescence. Compare the In-doped ZnO on Si substrate, the enhancement of PL intensity for In-doped ZnO with deposited Al pattern film can be attributed to strong interaction with SP resonance and exciton over a broad temperature range. These experimental results indicate that Al cylindrical micropillars can significantly enhance carrier confinement and increase the quantum efficiency of In-doped ZnO/Al heterostructures due to the interaction of SP resonance between the In-doped ZnO nanowires and Al cylindrical micropillar structures, the surface-defect related luminescence, and the auxiliary test structures with variable micropillar parameters. -- Highlights: ► We examine the exciton radiative recombination of the ZnO nanowires. ► Al cylindrical micropillars affect the carrier recombination of ZnO/Al structures. ► The interaction of SP resonance between In-doped ZnO nanowire and Al pattern film. ► The carrier

  17. Influence of excitonic effects on luminescence quantum yield in silicon

    Energy Technology Data Exchange (ETDEWEB)

    Sachenko, A.V.; Kostylyov, V.P.; Vlasiuk, V.M. [V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine, 41 prospect Nauky, 03028 Kyiv (Ukraine); Sokolovskyi, I.O., E-mail: isokolovskyi@mun.ca [V. Lashkaryov Institute of Semiconductor Physics, NAS of Ukraine, 41 prospect Nauky, 03028 Kyiv (Ukraine); Department of Physics and Physical Oceanography, Memorial University of Newfoundland, St. John' s, NL, A1B 3X7 Canada (Canada); Evstigneev, M. [Department of Physics and Physical Oceanography, Memorial University of Newfoundland, St. John' s, NL, A1B 3X7 Canada (Canada)

    2017-03-15

    Nonradiative exciton lifetime in silicon is determined by comparison of the experimental and theoretical curves of bulk minority charge carriers lifetime on doping and excitation levels. This value is used to analyze the influence of excitonic effects on internal luminescence quantum yield at room temperature, taking into account both nonradiative and radiative exciton lifetimes. A range of Shockley-Hall-Reed lifetimes is found, where excitonic effects lead to an increase of internal luminescence quantum yield.

  18. The nature of singlet excitons in oligoacene molecular crystals

    KAUST Repository

    Yamagata, H.; Norton, J.; Hontz, E.; Olivier, Y.; Beljonne, D.; Brédas, J. L.; Silbey, R. J.; Spano, F. C.

    2011-01-01

    A theory for polarized absorption in crystalline oligoacenes is presented, which includes Frenkel exciton coupling, the coupling between Frenkel and charge-transfer (CT) excitons, and the coupling of all neutral and ionic excited states to the dominant ring-breathing vibrational mode. For tetracene, spectra calculated using all Frenkel couplings among the five lowest energy molecular singlet states predict a Davydov splitting (DS) of the lowest energy (0-0) vibronic band of only -32cm-1, far smaller than the measured value of 631cm-1 and of the wrong sign-a negative sign indicating that the polarizations of the lower and upper Davydov components are reversed from experiment. Inclusion of Frenkel-CT coupling dramatically improves the agreement with experiment, yielding a 0-0 DS of 601cm-1 and a nearly quantitative reproduction of the relative spectral intensities of the 0-n vibronic components. Our analysis also shows that CT mixing increases with the size of the oligoacenes. We discuss the implications of these results on exciton dissociation and transport. © 2011 American Institute of Physics.

  19. Quasi-particle energies and optical excitations of hydrogenated and fluorinated germanene.

    Science.gov (United States)

    Shu, Huabing; Li, Yunhai; Wang, Shudong; Wang, Jinlan

    2015-02-14

    Using density functional theory, the G0W0 method and Bethe-Salpeter equation calculations, we systematically explore the structural, electronic and optical properties of hydrogenated and fluorinated germanene. The hydrogenated/fluorinated germanene tends to form chair and zigzag-line configurations and its electronic and optical properties show close geometry dependence. The chair hydrogenated/fluorinated and zigzag-line fluorinated germanene are direct band-gap semiconductors, while the zigzag-line hydrogenated germanene owns an indirect band-gap. Moreover, the quasi-particle corrections are significant and strong excitonic effects with large exciton binding energies are observed. Moreover, the zigzag-line hydrogenated/fluorinated germanene shows highly anisotropic optical responses, which may be used as a good optical linear polarizer.

  20. Spectral Barcoding of Quantum Dots: Deciphering Structural Motifs from the Excitonic Spectra

    International Nuclear Information System (INIS)

    Mlinar, V.; Zunger, A.

    2009-01-01

    Self-assembled semiconductor quantum dots (QDs) show in high-resolution single-dot spectra a multitude of sharp lines, resembling a barcode, due to various neutral and charged exciton complexes. Here we propose the 'spectral barcoding' method that deciphers structural motifs of dots by using such barcode as input to an artificial-intelligence learning system. Thus, we invert the common practice of deducing spectra from structure by deducing structure from spectra. This approach (i) lays the foundation for building a much needed structure-spectra understanding for large nanostructures and (ii) can guide future design of desired optical features of QDs by controlling during growth only those structural motifs that decide given optical features.

  1. Donor bound excitons in ZnSe nanoresonators - Applications in quantum information science

    Energy Technology Data Exchange (ETDEWEB)

    Pawlis, A. [Department of Physics, University of Paderborn, Warburger Str. 100, 33098 Paderborn, Germany and Edward L. Ginzton Laboratory, Stanford University, Stanford, California 94305-4088 (United States); Lischka, K. [Department of Physics, University of Paderborn, Warburger Str. 100, 33098 Paderborn (Germany); Sanaka, K.; Yamamoto, Y. [Edward L. Ginzton Laboratory, Stanford University, Stanford, California 94305-4088, USA and National Institute of Informatics, 2-1-2 Hitotsubashi, Chiyoda-ku, Tokyo 101-8430 (Japan); Sleiter, D. [Edward L. Ginzton Laboratory, Stanford University, Stanford, California 94305-4088 (United States)

    2014-05-15

    Here we summarize the advantages of excitons bound to isolated fluorine donor in ZnSe/ZnMgSe quantum well nano-structures. Devices based on these semiconductors, are particularly suited to implement concepts of the optical manipulation of quantum states in solid-state material. The fluorine donor in ZnSe provides a physical qubit with potential advantages over previously researched qubits. In this context we show several initial demonstrations of devices, such as a low-threshold microdisk laser and an indistinguishable single photon source. Additionally we demonstrate the realization of a controllable three-level-system qubit consisting of a single Fluorine donor in a ZnSe nano-pillar, which provides an optical accessible single electon spin qubit.

  2. Fractional Solitons in Excitonic Josephson Junctions

    Science.gov (United States)

    Su, Jung-Jung; Hsu, Ya-Fen

    The Josephson effect is especially appealing because it reveals macroscopically the quantum order and phase. Here we study this effect in an excitonic Josephson junction: a conjunct of two exciton condensates with a relative phase ϕ0 applied. Such a junction is proposed to take place in the quantum Hall bilayer (QHB) that makes it subtler than in superconductor because of the counterflow of excitonic supercurrent and the interlayer tunneling in QHB. We treat the system theoretically by first mapping it into a pseudospin ferromagnet then describing it by the Landau-Lifshitz-Gilbert equation. In the presence of interlayer tunneling, the excitonic Josephson junction can possess a family of fractional sine-Gordon solitons that resemble the static fractional Josephson vortices in the extended superconducting Josephson junctions. Interestingly, each fractional soliton carries a topological charge Q which is not necessarily a half/full integer but can vary continuously. The resultant current-phase relation (CPR) shows that solitons with Q =ϕ0 / 2 π are the lowest energy states for small ϕ0. When ϕ0 > π , solitons with Q =ϕ0 / 2 π - 1 take place - the polarity of CPR is then switched.

  3. Magnetic excitons in singlet-ground-state ferromagnets

    DEFF Research Database (Denmark)

    Birgeneau, R.J.; Als-Nielsen, Jens Aage; Bucher, E.

    1971-01-01

    The authors report measurements of the dispersion of singlet-triplet magnetic excitons as a function of temperature in the singlet-ground-state ferromagnets fcc Pr and Pr3Tl. Well-defined excitons are observed in both the ferromagnetic and paramagnetic regions, but with energies which are nearly...

  4. Exciton Transport Simulations in Phenyl Cored Thiophene Dendrimers

    Science.gov (United States)

    Kim, Kwiseon; Erkan Kose, Muhammet; Graf, Peter; Kopidakis, Nikos; Rumbles, Garry; Shaheen, Sean E.

    2009-03-01

    Phenyl cored 3-arm and 4-arm thiophene dendrimers are promising materials for use in photovoltaic devices. It is important to understand the energy transfer mechanisms in these molecules to guide the synthesis of novel dendrimers with improved efficiency. A method is developed to estimate the exciton diffusion lengths for the dendrimers and similar chromophores in amorphous films. The approach exploits Fermi's Golden Rule to estimate the energy transfer rates for an ensemble of bimolecular complexes in random orientations. Using Poisson's equation to evaluate Coulomb integrals led to efficient calculation of excitonic couplings between the transition densities. Monte-Carlo simulations revealed the dynamics of energy transport in the dendrimers. Experimental exciton diffusion lengths of the dendrimers range 10 ˜ 20 nm, increasing with the size of the dendrimer. Simulated diffusion lengths correlate well with experiments. The chemical structure of the chromophore, the shape of the transition densities and the exciton lifetime are found to be the most important factors that determine the exciton diffusion length in amorphous films.

  5. Electron Spin Optical Orientation in Charged Quantum Dots

    Science.gov (United States)

    Shabaev, A.; Gershoni, D.; Korenev, V. L.

    2005-03-01

    We present a theory of nonresonant optical orientation of electron spins localized in quantum dots. This theory explains the negative circularly polarized photoluminescence of singlet trions localized in quantum dots previously observed in experiments where trion polarization changed to negative with time and where the degree of the negative polarization increased with intensity of pumping light. We have shown that this effect can be explained by the accumulation of dark excitons that occurs due to the spin blocking of the singlet trion formation - the major mechanism of dark exciton recombination. The accumulation of dark excitons results from a lack of electrons with a spin matching the exciton polarization. The electron spin lifetime is shortened by a transverse magnetic field or a temperature increase. This takes the block off the dark exciton recombination and restores the positive degree of trion polarization. The presented theory gives good agreement with experimental data.

  6. Theory for electric dipole superconductivity with an application for bilayer excitons.

    Science.gov (United States)

    Jiang, Qing-Dong; Bao, Zhi-qiang; Sun, Qing-Feng; Xie, X C

    2015-07-08

    Exciton superfluid is a macroscopic quantum phenomenon in which large quantities of excitons undergo the Bose-Einstein condensation. Recently, exciton superfluid has been widely studied in various bilayer systems. However, experimental measurements only provide indirect evidence for the existence of exciton superfluid. In this article, by viewing the exciton in a bilayer system as an electric dipole, we derive the London-type and Ginzburg-Landau-type equations for the electric dipole superconductors. By using these equations, we discover the Meissner-type effect and the electric dipole current Josephson effect. These effects can provide direct evidence for the formation of the exciton superfluid state in bilayer systems and pave new ways to drive an electric dipole current.

  7. Nonlinear optical characteristics of monolayer MoSe{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Le, Chinh Tam; Ullah, Farman; Senthilkumar, Velusamy; Kim, Yong Soo [Department of Physics and Energy Harvest Storage Research Center, University of Ulsan (Korea, Republic of); Clark, Daniel J.; Jang, Joon I. [Department of Physics, Applied Physics and Astronomy, Binghamton University, Binghamton, NY (United States); Sim, Yumin; Seong, Maeng-Je [Department of Physics, Chung-Ang University, Seoul (Korea, Republic of); Chung, Koo-Hyun [School of Mechanical Engineering, University of Ulsan (Korea, Republic of); Park, Hyoyeol [Electronics, Communication and Semiconductor Applications Department, Ulsan College (Korea, Republic of)

    2016-08-15

    In this study, we utilized picosecond pulses from an Nd:YAG laser to investigate the nonlinear optical characteristics of monolayer MoSe{sub 2}. Two-step growth involving the selenization of pulsed-laser-deposited MoO{sub 3} film was employed to yield the MoSe{sub 2} monolayer on a SiO{sub 2}/Si substrate. Raman scattering, photoluminescence (PL) spectroscopy, and atomic force microscopy verified the high optical quality of the monolayer. The second-order susceptibility χ{sup (2)} was calculated to be ∝50 pm V{sup -1} at the second harmonic wavelength λ{sub SHG} ∝810 nm, which is near the optical gap of the monolayer. Interestingly, our wavelength-dependent second harmonic scan can identify the bound excitonic states including negatively charged excitons much more efficiently, compared with the PL method at room temperature. Additionally, the MoSe{sub 2} monolayer exhibits a strong laser-induced damage threshold ∝16 GW cm{sup -2} under picosecond-pulse excitation{sub .} Our findings suggest that monolayer MoSe{sub 2} can be considered as a promising candidate for high-power, thin-film-based nonlinear optical devices and applications. (copyright 2016 by WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  8. Optical investigation of carrier tunneling in semiconductor nanostructures

    Science.gov (United States)

    Emiliani, V.; Ceccherini, S.; Bogani, F.; Colocci, M.; Frova, A.; Shi, Song Stone

    1997-08-01

    The tunneling dynamics of excitons and free carriers in AlxGa1-xAs/GaAs asymmetric double quantum well and near-surface quantum well structures has been investigated by means of time-resolved optical techniques. The competing processes of carrier tunneling out of the quantum well and exciton formation and recombination inside the quantum well have been thoroughly studied in the range of the excitation densities relevant to device applications. A consistent picture capable of fully describing the carrier and exciton-tunneling mechanisms in both types of structures has been obtained and apparently contrasting results in the recent literature are clarified.

  9. Hopping approach towards exciton dissociation in conjugated polymers

    International Nuclear Information System (INIS)

    Emelianova, E. V.; Auweraer, M. van der; Baessler, H.

    2008-01-01

    By employing random walk an analytic theory for the dissociation of singlet excitons in a random organic solid, for instance, a conjugated polymer, has been developed. At variance of conventional three-dimensional Onsager theory, it is assumed that an exciton with finite lifetime can first transfer endothermically an electron to an adjacent site, thereby generating a charge transfer state whose energy is above the energy of that of the initial exciton. In a second step the latter can fully dissociate in accordance with Onsager's concept Brownian motion. The results indicate that, depending of the energy required for the first jump, the first jump contributes significantly to the field dependence of the dissociation yield. Disorder weakens the temperature dependence of the yield dramatically and precludes extracting information on the exciton binding energy from it

  10. 4P-NPD ultra thin-films as efficient exciton blocking layers in DBP/C70 based organic solar cells

    DEFF Research Database (Denmark)

    Patil, Bhushan Ramesh; Liu, Yiming; Qamar, Talha

    2017-01-01

    Exciton blocking effects from ultra thin layers of N,N'-di-1-naphthalenyl-N,N'-diphenyl [1,1':4',1'':4'',1'''-quaterphenyl]-4,4'''-diamine (4P-NPD) was investigated in small molecule based inverted Organic Solar Cells (OSCs) using Tetraphenyldibenzoperiflanthene (DBP) as the electron donor material...... and fullerene (C70) as the electron acceptor material. The short-circuit current density (Jsc) and PCE of the optimized OSCs with 0.7 nm thick 4P-NPD were approx. 16 % and 24 % higher, respectively, compared to reference devices without exciton blocking layers. Drift diffusion based device modeling...... was conducted to model the full Current density – Voltage (JV) characteristics and EQE spectrum of the OSCs, and photoluminescence measurements was conducted to investigate the exciton blocking effects with increasing thicknesses of the 4P-NPD layer. Importantly, coupled optical and electrical modeling studies...

  11. Direct determination of monolayer MoS2 and WSe2 exciton binding energies on insulating and metallic substrates

    KAUST Repository

    Park, Soohyung; Mutz, Niklas; Schultz, Thorsten; Blumstengel, Sylke; Han, Ali; Aljarb, Areej; Li, Lain-Jong; List-Kratochvil, Emil J W; Amsalem, Patrick; Koch, Norbert

    2018-01-01

    Understanding the excitonic nature of excited states in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) is of key importance to make use of their optical and charge transport properties in optoelectronic applications. We contribute to this by the direct experimental determination of the exciton binding energy (E b,exc) of monolayer MoS2 and WSe2 on two fundamentally different substrates, i.e. the insulator sapphire and the metal gold. By combining angle-resolved direct and inverse photoelectron spectroscopy we measure the electronic band gap (E g), and by reflectance measurements the optical excitonic band gap (E exc). The difference of these two energies is E b,exc. The values of E g and E b,exc are 2.11 eV and 240 meV for MoS2 on sapphire, and 1.89 eV and 240 meV for WSe2 on sapphire. On Au E b,exc is decreased to 90 meV and 140 meV for MoS2 and WSe2, respectively. The significant E b,exc reduction is primarily due to a reduction of E g resulting from enhanced screening by the metal, while E exc is barely decreased for the metal support. Energy level diagrams determined at the K-point of the 2D TMDCs Brillouin zone show that MoS2 has more p-type character on Au as compared to sapphire, while WSe2 appears close to intrinsic on both. These results demonstrate that the impact of the dielectric environment of 2D TMDCs is more pronounced for individual charge carriers than for a correlated electron–hole pair, i.e. the exciton. A proper dielectric surrounding design for such 2D semiconductors can therefore be used to facilitate superior optoelectronic device function.

  12. Direct determination of monolayer MoS2 and WSe2 exciton binding energies on insulating and metallic substrates

    Science.gov (United States)

    Park, Soohyung; Mutz, Niklas; Schultz, Thorsten; Blumstengel, Sylke; Han, Ali; Aljarb, Areej; Li, Lain-Jong; List-Kratochvil, Emil J. W.; Amsalem, Patrick; Koch, Norbert

    2018-04-01

    Understanding the excitonic nature of excited states in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) is of key importance to make use of their optical and charge transport properties in optoelectronic applications. We contribute to this by the direct experimental determination of the exciton binding energy (E b,exc) of monolayer MoS2 and WSe2 on two fundamentally different substrates, i.e. the insulator sapphire and the metal gold. By combining angle-resolved direct and inverse photoelectron spectroscopy we measure the electronic band gap (E g), and by reflectance measurements the optical excitonic band gap (E exc). The difference of these two energies is E b,exc. The values of E g and E b,exc are 2.11 eV and 240 meV for MoS2 on sapphire, and 1.89 eV and 240 meV for WSe2 on sapphire. On Au E b,exc is decreased to 90 meV and 140 meV for MoS2 and WSe2, respectively. The significant E b,exc reduction is primarily due to a reduction of E g resulting from enhanced screening by the metal, while E exc is barely decreased for the metal support. Energy level diagrams determined at the K-point of the 2D TMDCs Brillouin zone show that MoS2 has more p-type character on Au as compared to sapphire, while WSe2 appears close to intrinsic on both. These results demonstrate that the impact of the dielectric environment of 2D TMDCs is more pronounced for individual charge carriers than for a correlated electron-hole pair, i.e. the exciton. A proper dielectric surrounding design for such 2D semiconductors can therefore be used to facilitate superior optoelectronic device function.

  13. Direct determination of monolayer MoS2 and WSe2 exciton binding energies on insulating and metallic substrates

    KAUST Repository

    Park, Soohyung

    2018-01-03

    Understanding the excitonic nature of excited states in two-dimensional (2D) transition-metal dichalcogenides (TMDCs) is of key importance to make use of their optical and charge transport properties in optoelectronic applications. We contribute to this by the direct experimental determination of the exciton binding energy (E b,exc) of monolayer MoS2 and WSe2 on two fundamentally different substrates, i.e. the insulator sapphire and the metal gold. By combining angle-resolved direct and inverse photoelectron spectroscopy we measure the electronic band gap (E g), and by reflectance measurements the optical excitonic band gap (E exc). The difference of these two energies is E b,exc. The values of E g and E b,exc are 2.11 eV and 240 meV for MoS2 on sapphire, and 1.89 eV and 240 meV for WSe2 on sapphire. On Au E b,exc is decreased to 90 meV and 140 meV for MoS2 and WSe2, respectively. The significant E b,exc reduction is primarily due to a reduction of E g resulting from enhanced screening by the metal, while E exc is barely decreased for the metal support. Energy level diagrams determined at the K-point of the 2D TMDCs Brillouin zone show that MoS2 has more p-type character on Au as compared to sapphire, while WSe2 appears close to intrinsic on both. These results demonstrate that the impact of the dielectric environment of 2D TMDCs is more pronounced for individual charge carriers than for a correlated electron–hole pair, i.e. the exciton. A proper dielectric surrounding design for such 2D semiconductors can therefore be used to facilitate superior optoelectronic device function.

  14. Organic-Inorganic Composites of Semiconductor Nanocrystals for Efficient Excitonics.

    Science.gov (United States)

    Guzelturk, Burak; Demir, Hilmi Volkan

    2015-06-18

    Nanocomposites of colloidal semiconductor nanocrystals integrated into conjugated polymers are the key to soft-material hybrid optoelectronics, combining advantages of both plastics and particles. Synergic combination of the favorable properties in the hybrids of colloidal nanocrystals and conjugated polymers offers enhanced performance and new functionalities in light-generation and light-harvesting applications, where controlling and mastering the excitonic interactions at the nanoscale are essential. In this Perspective, we highlight and critically consider the excitonic interactions in the organic-inorganic nanocomposites to achieve highly efficient exciton transfer through rational design of the nanocomposites. The use of strong excitonic interactions in optoelectronic devices can trigger efficiency breakthroughs in hybrid optoelectronics.

  15. Resonant transfer of excitons and quantum computation

    International Nuclear Information System (INIS)

    Lovett, Brendon W.; Reina, John H.; Nazir, Ahsan; Kothari, Beeneet; Briggs, G. Andrew D.

    2003-01-01

    Resonant energy transfer mechanisms have been observed in the sensitized luminescence of solids, and in quantum dots, molecular nanostructures, and photosynthetic organisms. We demonstrate that such mechanisms, together with the exciton-exciton binding energy shift typical of these nanostructures, can be used to perform universal quantum logic and generate quantum entanglement

  16. Exciton dephasing in ZnSe quantum wires

    DEFF Research Database (Denmark)

    Wagner, Hans Peter; Langbein, Wolfgang Werner; Hvam, Jørn Märcher

    1998-01-01

    The homogeneous linewidths of excitons in wet-etched ZnSe quantum wires of lateral sizes down to 23 nm are studied by transient four-wave mixing. The low-density dephasing time is found to increase with decreasing wire width. This is attributed mainly to a reduction of electron-exciton scattering...

  17. Single-shot quantum nondemolition measurement of a quantum-dot electron spin using cavity exciton-polaritons

    Science.gov (United States)

    Puri, Shruti; McMahon, Peter L.; Yamamoto, Yoshihisa

    2014-10-01

    We propose a scheme to perform single-shot quantum nondemolition (QND) readout of the spin of an electron trapped in a semiconductor quantum dot (QD). Our proposal relies on the interaction of the QD electron spin with optically excited, quantum well (QW) microcavity exciton-polaritons. The spin-dependent Coulomb exchange interaction between the QD electron and cavity polaritons causes the phase and intensity response of left circularly polarized light to be different than that of right circularly polarized light, in such a way that the QD electron's spin can be inferred from the response to a linearly polarized probe reflected or transmitted from the cavity. We show that with careful device design it is possible to essentially eliminate spin-flip Raman transitions. Thus a QND measurement of the QD electron spin can be performed within a few tens of nanoseconds with fidelity ˜99.95%. This improves upon current optical QD spin readout techniques across multiple metrics, including speed and scalability.

  18. Ultraviolet lasing behavior in ZnO optical microcavities

    Directory of Open Access Journals (Sweden)

    Hongxing Dong

    2017-12-01

    Full Text Available Zinc oxide (ZnO optical microcavity modulated UV lasers have been attracting a wide range of research interests. As one of the most important materials in developing high quality microcavity and efficient UV–visible optoelectronic devices due to its wide band gap (3.37 eV and large exciton binding energy (∼60 meV. In this review, we summarized the latest development of ZnO optical cavity based microlasers, mainly including Fabry-Perot mode lasers and whispering gallery mode lasers. The synthesis and optical studies of ZnO optical microcavities with different morphologies were discussed in detail. Finally, we also consider that the research focus in the near future would include new nanotechnology and physical effects, such as nano/micro fabrication, surface plasmon enhancement, and quantum dot coupling, which may result in new and interesting physical phenomena.

  19. Fluorescence Spectroscopy, Exciton Dynamics and Photochemistry of Single Allophycocyanin Trimers

    International Nuclear Information System (INIS)

    Ying, Liming; Xie, Xiaoliang

    1998-01-01

    We report a study of the spectroscopy and exciton dynamics of the allophycocyanin trimer (APC), a light harvesting protein complex from cyanobacteria, by room-temperature single-molecule measurements of fluorescence spectra, lifetimes, intensity trajectories and polarization modulation. Emission spectra of individual APC trimers are found to be homogeneous on the time scale of seconds. In contrast, their emission lifetimes are found to be widely distributed, because of generation of exciton traps during the course of measurements. The intensity trajectories and polarization modulation experiments indicate reversible ixciton trap formation within the three quasi-independent pairs of strong interacting a84 and B84 chromophores in APC, as well a photobleaching of individual chromophores. Comparison experiments under continuous wave and pulsed excitation reveal a two-photon mechanism for generating exciton traps and/or photobleaching, which involves exciton-exciton annihilation. These single-molecule experiments provide new insights into exciton dynamics and photochemistry of light-harvesting complexes

  20. Transport Gap and exciton binding energy determination in organic semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Krause, Stefan; Schoell, Achim; Reinert, Friedrich; Umbach, Eberhard [University of Wuerzburg (Germany). Experimental Physics II; Casu, Benedetta [Inst. f. Physik. u. Theor. Chemie, Tuebingen (Germany)

    2008-07-01

    The transport gap of an organic semiconductor is defined as the energy difference between the HOMO and LUMO levels in the presence of a hole or electron, respectively, after relaxation has occurred. Its knowledge is mandatory for the optimisation of electronic devices based on these materials. UV photoelectron spectroscopy (UPS) and inverse photoelectron spectroscopy (IPES) are routinely applied to measure these molecular levels. However, the precise determination of the transport gap on the basis of the respective data is not an easy task. It involves fundamental questions about the properties of organic molecules and their condensates, about their reaction on the experimental probe, and on the evaluation of the spectroscopic data. In particular electronic relaxation processes, which occur on the time scale of the photo excitation, have to be considered adequately. We determined the transport gap for the organic semiconductors PTCDA, Alq3, DIP, CuPc, and PBI-H4. After careful data analysis and comparison to the respective values for the optical gap we obtain values for the exciton binding energies between 0.1-0.5 eV. This is considerably smaller than commonly believed and indicates a significant delocalisation of the excitonic charge over various molecular units.

  1. Evolution of excitonic states in two-phase systems with quantum dots of II-VI semiconductors near the percolation threshold

    Science.gov (United States)

    Bondar, N. V.; Brodyn, M. S.

    2010-03-01

    In two-phase disordered media composed of borosilicate glass with ZnSe or CdS quantum dots, the formation of a phase percolation transition of carriers for near-threshold concentrations that are manifested in optical spectra has been observed. Microscopic fluctuations of the quantum-dot density near the percolation threshold were found that resembled the phenomenon of critical opalescence, where similar fluctuations of the density of a pure substance appear near to a phase transition. It is proposed that the dielectric mismatch between a matrix and ZnSe or CdS quantum dots plays a significant role in the carrier (exciton) delocalization, resulting in the appearance of a “dielectric Coulomb trap” beyond the QD border and the formation of surface states of excitons. The spatial overlapping of excitonic states at the critical density of quantum dots results in a tunneling of carriers and the formation of a phase percolation transition in such media.

  2. Photoluminescence dynamics of weakly confined excitons in GaAs thin films

    International Nuclear Information System (INIS)

    Kanno, Atsushi; Katouf, Redouane; Kojima, Osamu; Ishi-Hayase, Junko; Sasaki, Masahide; Tsuchiya, Masahiro; Isu, Toshiro

    2008-01-01

    We investigate the dynamics of weakly confined excitons in GaAs thin films measured by time-resolved photoluminescence (PL) technique. When excitation energy was above the resonant energy of the exciton, a long PL rise time of about 200 ps was observed. It is considered that an exciton formation process from excited continuum energy states to discrete energy states of the exciton in the thin film causes the slow PL rise. The observed PL decay time constant was about 14 ns due to high quality fabricated samples. The observed population dynamics can be surely ascribed to the specific features of weakly confined excitons

  3. Tailorable Exciton Transport in Doped Peptide–Amphiphile Assemblies

    Energy Technology Data Exchange (ETDEWEB)

    Solomon, Lee A. [Center; Sykes, Matthew E. [Center; Wu, Yimin A. [Center; Schaller, Richard D. [Center; Department; Wiederrecht, Gary P. [Center; Fry, H. Christopher [Center

    2017-08-29

    Light-harvesting biomaterials are an attractive target in photovoltaics, photocatalysis, and artificial photosynthesis. Through peptide self-assembly, complex nanostructures can be engineered to study the role of chromophore organization during light absorption and energy transport. To this end, we demonstrate the one-dimensional transport of excitons along naturally occurring, light-harvesting, Zn-protoporphyrin IX chromophores within self-assembled peptide-amphiphile nanofibers. The internal structure of the nanofibers induces packing of the porphyrins into linear chains. We find that this peptide assembly can enable long-range exciton diffusion, yet it also induces the formation of excimers between adjacent molecules, which serve as exciton traps. Electronic coupling between neighboring porphyrin molecules is confirmed by various spectroscopic methods. The exciton diffusion process is then probed through transient photoluminescence and absorption measurements and fit to a model for one-dimensional hopping. Because excimer formation impedes exciton hopping, increasing the interchromophore spacing allows for improved diffusivity, which we control through porphyrin doping levels. We show that diffusion lengths of over 60 nm are possible at low porphyrin doping, representing an order of magnitude improvement over the highest doping fractions.

  4. Molecular plasmonics: The role of rovibrational molecular states in exciton-plasmon materials under strong-coupling conditions

    Science.gov (United States)

    Sukharev, Maxim; Charron, Eric

    2017-03-01

    We extend the model of exciton-plasmon materials to include a rovibrational structure of molecules using wave-packet propagations on electronic potential energy surfaces. Our model replaces conventional two-level emitters with more complex molecules, allowing us to examine the influence of alignment and vibrational dynamics on strong coupling with surface plasmon-polaritons. We apply the model to a hybrid system comprising a thin layer of molecules placed on top of a periodic array of slits. Rigorous simulations are performed for two types of molecular systems described by vibrational bound-bound and bound-continuum electronic transitions. Calculations reveal new features in transmission, reflection, and absorption spectra, including the observation of significantly higher values of the Rabi splitting and vibrational patterns clearly seen in the corresponding spectra. We also examine the influence of anisotropic initial conditions on optical properties of hybrid materials, demonstrating that the optical response of the system is significantly affected by an initial prealignment of the molecules. Our work demonstrates that prealigned molecules could serve as an efficient probe for the subdiffraction characterization of the near-field near metal interfaces.

  5. Excitonic AND Logic Gates on DNA Brick Nanobreadboards

    Science.gov (United States)

    2015-01-01

    A promising application of DNA self-assembly is the fabrication of chromophore-based excitonic devices. DNA brick assembly is a compelling method for creating programmable nanobreadboards on which chromophores may be rapidly and easily repositioned to prototype new excitonic devices, optimize device operation, and induce reversible switching. Using DNA nanobreadboards, we have demonstrated each of these functions through the construction and operation of two different excitonic AND logic gates. The modularity and high chromophore density achievable via this brick-based approach provide a viable path toward developing information processing and storage systems. PMID:25839049

  6. Radiative recombination of excitons in amorphous semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Singh, Jai [School of Engineering and Logistics, Faculty Technology, B-41, Charles Darwin University, Darwin, NT 0909 (Australia)]. E-mail: jai.singh@cdu.edu.au

    2005-04-15

    A theory for calculating the radiative lifetime of excitons in amorphous semiconductors is presented. Four possibilities of excitonic radiative recombination are considered and the corresponding rates are derived at thermal equilibrium. The radiative lifetime is calculated from the inverse of the maximum rate for all the four possibilities. Results agree very well with experiments.

  7. Radiative recombination of excitons in amorphous semiconductors

    International Nuclear Information System (INIS)

    Singh, Jai

    2005-01-01

    A theory for calculating the radiative lifetime of excitons in amorphous semiconductors is presented. Four possibilities of excitonic radiative recombination are considered and the corresponding rates are derived at thermal equilibrium. The radiative lifetime is calculated from the inverse of the maximum rate for all the four possibilities. Results agree very well with experiments

  8. Spatial mapping of exciton lifetimes in single ZnO nanowires

    Directory of Open Access Journals (Sweden)

    J. S. Reparaz

    2013-07-01

    Full Text Available We investigate the spatial dependence of the exciton lifetimes in single ZnO nanowires. We have found that the free exciton and bound exciton lifetimes exhibit a maximum at the center of nanowires, while they decrease by 30% towards the tips. This dependence is explained by considering the cavity-like properties of the nanowires in combination with the Purcell effect. We show that the lifetime of the bound-excitons scales with the localization energy to the power of 3/2, which validates the model of Rashba and Gurgenishvili at the nanoscale.

  9. Molecular weight dependence of exciton diffusion in poly(3-hexylthiophene)

    DEFF Research Database (Denmark)

    Masri, Zarifi; Ruseckas, Arvydas; Emelianova, Evguenia V.

    2013-01-01

    A joint experimental and theoretical study of singlet exciton diffusion in spin-coated poly(3-hexylthiophene) (P3HT) films and its dependence on molecular weight is presented. The results show that exciton diffusion is fast along the co-facial π–π aggregates of polymer chromophores and about 100...... times slower in the lateral direction between aggregates. Exciton hopping between aggregates is found to show a subtle dependence on interchain coupling, aggregate size, and Boltzmann statistics. Additionally, a clear correlation is observed between the effective exciton diffusion coefficient...

  10. PREFACE: Ultrafast and nonlinear optics in carbon nanomaterials

    Science.gov (United States)

    Kono, Junichiro

    2013-02-01

    Carbon-based nanomaterials—single-wall carbon nanotubes (SWCNTs) and graphene, in particular—have emerged in the last decade as novel low-dimensional systems with extraordinary properties. Because they are direct-bandgap systems, SWCNTs are one of the leading candidates to unify electronic and optical functions in nanoscale circuitry; their diameter-dependent bandgaps can be utilized for multi-wavelength devices. Graphene's ultrahigh carrier mobilities are promising for high-frequency electronic devices, while, at the same time, it is predicted to have ideal properties for terahertz generation and detection due to its unique zero-gap, zero-mass band structure. There have been a large number of basic optical studies on these materials, but most of them were performed in the weak-excitation, quasi-equilibrium regime. In order to probe and assess their performance characteristics as optoelectronic materials under device-operating conditions, it is crucial to strongly drive them and examine their optical properties in highly non-equilibrium situations and with ultrashot time resolution. In this section, the reader will find the latest results in this rapidly growing field of research. We have assembled contributions from some of the leading experts in ultrafast and nonlinear optical spectroscopy of carbon-based nanomaterials. Specific topics featured include: thermalization, cooling, and recombination dynamics of photo-generated carriers; stimulated emission, gain, and amplification; ultrafast photoluminescence; coherent phonon dynamics; exciton-phonon and exciton-plasmon interactions; exciton-exciton annihilation and Auger processes; spontaneous and stimulated emission of terahertz radiation; four-wave mixing and harmonic generation; ultrafast photocurrents; the AC Stark and Franz-Keldysh effects; and non-perturbative light-mater coupling. We would like to express our sincere thanks to those who contributed their latest results to this special section, and the

  11. Pool-Frenkel thermoelectric modulation of exciton photoluminescence in GaSe crystals

    International Nuclear Information System (INIS)

    Ertap, H.; Mamedov, G.M.; Karabulut, M.; Bacioglu, A.

    2011-01-01

    Effect of external field on the exciton photoluminescence of GaSe crystals has been investigated and it has been observed that the PL is quenched with the applied field. The changes observed in the PL spectra have been analyzed with impact exciton, Franz-Keldysh and Pool-Frenkel effects. From the analyses of the experimental data, it has been found that the intensity of direct free, indirect free and bound exciton peaks decreased exponentially with the square root of applied field as I∼exp-β√E. The energy positions of emission peaks were found to shift to longer wavelength with the applied field as ΔE∼β√E. From these findings, the Pool-Frenkel thermoelectric field effect is seen to be the dominant mechanism in the variation of exciton PL with the applied field even though the impact exciton and Franz-Keldysh effects contribute. - Highlights: → Exciton PL intensity varies with the applied field. It decreases with the square root of E in accordance with Pool-Frenkel effect. → In the intrinsic region of PL spectrum, lines belonging to direct and indirect free/bound excitons were observed. → Line positions shifted to longer wavelengths with the applied field. → It was shown that amplitude modulation of exciton PL with electric field was possible.

  12. Strong excitonic interactions in the oxygen K-edge of perovskite oxides

    Energy Technology Data Exchange (ETDEWEB)

    Tomita, Kota; Miyata, Tomohiro [Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo 153-8505 (Japan); Olovsson, Weine [Department of Physics, Chemistry and Biology (IFM), Linköping University, SE-581 83 Linköping (Sweden); Mizoguchi, Teruyasu, E-mail: teru@iis.u-tokyo.ac.jp [Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo 153-8505 (Japan)

    2017-07-15

    Excitonic interactions of the oxygen K-edge electron energy-loss near-edge structure (ELNES) of perovskite oxides, CaTiO{sub 3}, SrTiO{sub 3}, and BaTiO{sub 3}, together with reference oxides, MgO, CaO, SrO, BaO, and TiO{sub 2}, were investigated using a first-principles Bethe–Salpeter equation calculation. Although the transition energy of oxygen K-edge is high, strong excitonic interactions were present in the oxygen K-edge ELNES of the perovskite oxides, whereas the excitonic interactions were negligible in the oxygen K-edge ELNES of the reference compounds. Detailed investigation of the electronic structure suggests that the strong excitonic interaction in the oxygen K-edge ELNES of the perovskite oxides is caused by the directionally confined, low-dimensional electronic structure at the Ti–O–Ti bonds. - Highlights: • Excitonic interaction in oxygen-K edge is investigated. • Strong excitonic interaction is found in the oxygen-K edge of perovskite oxides. • The strong excitonic interaction is ascribed to the low-dimensional and confined electronic structure.

  13. Strongly Enhanced Free-Exciton Luminescence in Microcrystalline CsPbBr3 Films

    Science.gov (United States)

    Kondo, Shin-ichi; Kakuchi, Mitsugu; Masaki, Atsushi; Saito, Tadaaki

    2003-07-01

    The luminescence properties of CsPbBr3 films prepared via the amorphous phase by crystallization are dominated by free-exciton emission, and only a weak trace of emission due to trapped excitons was observed, in contrast to the case of bulk CsPbBr3 crystals. In particular, the films in the microcrystalline state show by more than an order of magnitude stronger free-exciton emission than in the polycrystalline state. The enhanced free-exciton emission is suggestive of excitonic superradiance.

  14. Extension of the radiative lifetime of Wannier-Mott excitons in semiconductor nanoclusters

    International Nuclear Information System (INIS)

    Kukushkin, V. A.

    2015-01-01

    The purpose of the study is to calculate the radiative lifetime of Wannier-Mott excitons in three-dimensional potential wells formed of direct-gap narrow-gap semiconductor nanoclusters in wide-gap semiconductors and assumed to be large compared to the exciton radius. Calculations are carried out for the InAs/GaAs heterosystem. It is shown that, as the nanocluster dimensions are reduced to values on the order of the exciton radius, the exciton radiative lifetime becomes several times longer compared to that in a homogeneous semiconductor. The increase in the radiative lifetime is more pronounced at low temperatures. Thus, it is established that the placement of Wannier-Mott excitons into direct-gap semiconductor nanoclusters, whose dimensions are of the order of the exciton radius, can be used for considerable extension of the exciton radiative lifetime

  15. Exciton states in GaAs δ-doped systems under magnetic fields and hydrostatic pressure

    Energy Technology Data Exchange (ETDEWEB)

    Mora-Ramos, M.E. [Facultad de Ciencias, Universidad Autónoma del Estado de Morelos, Ave. Universidad 1001, CP 62209 Cuernavaca, Morelos (Mexico); Instituto de Física, Universidad de Antioquia, AA 1226 Medellín (Colombia); Duque, C.A., E-mail: cduque@fisica.udea.edu.co [Instituto de Física, Universidad de Antioquia, AA 1226 Medellín (Colombia)

    2013-04-15

    Excitons in GaAs n-type δ-doped quantum wells are studied taking into account the effects of externally applied magnetic fields as well as of hydrostatic pressure. The one-dimensional potential profile in both the conduction and valence bands is described including Hartree effects via a Thomas–Fermi-based local density approximation. The allowed uncorrelated energy levels are calculated within the effective mass and envelope function approximations by means of an expansion over an orthogonal set of infinite well eigenfunctions and a variational method is used to obtain the exciton states. The results are presented as functions of the two-dimensional doping concentration and the magnetic field strength for zero and finite values of the hydrostatic pressure. In general, it is found that the exciton binding energy is a decreasing function of the doping-density and an increasing function of the magnetic field intensity. A comparison with recent experiments on exciton-related photoluminescence in n-type δ-doped GaAs is made.

  16. Exciton in type-II quantum dot

    Energy Technology Data Exchange (ETDEWEB)

    Sierra-Ortega, J; Escorcia, R A [Universidad del Magdalena, A. A. 731, Santa Marta (Colombia); Mikhailov, I D, E-mail: jsierraortega@gmail.co [Universidad Industrial de Santander, A. A. 678, Bucaramanga (Colombia)

    2009-05-01

    We study the quantum-size effect and the influence of the external magnetic field on the exciton ground state energy in the type-II InP quantum disk, lens and pyramid deposited on a wetting layer and embedded in a GaInP matrix. We show that the charge distribution over and below quantum dot and wetting layer induced by trapped exciton strongly depends on the quantum dot morphology and the strength of the magnetic field.

  17. Radiative recombination process of high density excitons in CdS crystals

    Energy Technology Data Exchange (ETDEWEB)

    Dneprovskij, V.S.; Klimov, V.I.; Martynenko, E.D.; Stadnik, V.A.

    1983-11-01

    The behaviour of the P-, E-, L- and Q-lines of luminescence in CdS is compared with calculated results for the processes of exciton-exciton scattering, exciton-electron scattering, annihilation of equilibrium electron-hole fluid (EHF), annihilation of electron-hole plasma (processes of amplification and reabsorption are taken into account). The comparison permitted to determine parameters of high density exciton gas and EHF. Spectral-kinetic properties of generation are investigated, and amplification factor in CdS is estimated.

  18. Comment on 'Unconventional gap state of trapped exciton in lead sulfide quantum dots'

    Energy Technology Data Exchange (ETDEWEB)

    Curry, R J, E-mail: r.j.curry@surrey.ac.uk [Advanced Technology Institute, University of Surrey, Guildford, Surrey, GU2 7XH (United Kingdom)

    2011-06-10

    In a recent paper (Lewis et al 2010 Nanotechnology 21 45502) proposed a previously unidentified gap state within lead sulfide nanocrystals (PbS-NCs) based on analysis of their temperature dependent optical properties. In the following we argue that due to oversights in the analysis of the data presented, inconsistencies arise which question their exclusion of 'dark' excitonic states as the origin of the observed effects. (comment)

  19. Excitons in InP/InAs inhomogeneous quantum dots

    CERN Document Server

    Assaid, E; Khamkhami, J E; Dujardin, F

    2003-01-01

    Wannier excitons confined in an InP/InAs inhomogeneous quantum dot (IQD) have been studied theoretically in the framework of the effective mass approximation. A finite-depth potential well has been used to describe the effect of the quantum confinement in the InAs layer. The exciton binding energy has been determined using the Ritz variational method. The spatial correlation between the electron and the hole has been taken into account in the expression for the wavefunction. It has been shown that for a fixed size b of the IQD, the exciton binding energy depends strongly on the core radius a. Moreover, it became apparent that there are two critical values of the core radius, a sub c sub r sub i sub t and a sub 2 sub D , for which important changes of the exciton binding occur. The former critical value, a sub c sub r sub i sub t , corresponds to a minimum of the exciton binding energy and may be used to distinguish between tridimensional confinement and bidimensional confinement. The latter critical value, a ...

  20. Inverse Funnel Effect of Excitons in Strained Black Phosphorus

    Directory of Open Access Journals (Sweden)

    Pablo San-Jose

    2016-09-01

    Full Text Available We study the effects of strain on the properties and dynamics of Wannier excitons in monolayer (phosphorene and few-layer black phosphorus (BP, a promising two-dimensional material for optoelectronic applications due to its high mobility, mechanical strength, and strain-tunable direct band gap. We compare the results to the case of molybdenum disulphide (MoS_{2} monolayers. We find that the so-called funnel effect, i.e., the possibility of controlling exciton motion by means of inhomogeneous strains, is much stronger in few-layer BP than in MoS_{2} monolayers and, crucially, is of opposite sign. Instead of excitons accumulating isotropically around regions of high tensile strain like in MoS_{2}, excitons in BP are pushed away from said regions. This inverse funnel effect is moreover highly anisotropic, with much larger funnel distances along the armchair crystallographic direction, leading to a directional focusing of exciton flow. A strong inverse funnel effect could enable simpler designs of funnel solar cells and offer new possibilities for the manipulation and harvesting of light.

  1. Electronic and optical properties of bilayer PbI2: a first-principles study

    Science.gov (United States)

    Shen, Chenhai; Wang, Guangtao

    2018-01-01

    By employing first-principles methods, we investigate the effects of stacking patterns and interlayer coupling on the electronic structures and optical properties of bilayer (BL) PbI2. For optical properties, excitonic effects are considered. The results show that crystal-type BL PbI2 stacking pattern is the most stable bilayer structures with the equilibrium interlayer distance of 3.27 Å and a direct band structure. Moreover, for all considered patterns, the interlayer coupling can induce the band structures to transform from indirect to direct and also the band gap values to vary from 2.56 eV to 2.62 eV. In addition, our calculations show that the exciton binding energy of the most stable pattern is 0.81 eV, and excitonic effects have obvious influences on optical responses of BL PbI2. These results may be useful to future experimental studies on optoelectronic properties of two-dimensional BL PbI2 nanosheets.

  2. Coherently-enabled environmental control of optics and energy transfer pathways of hybrid quantum dot-metallic nanoparticle systems.

    Science.gov (United States)

    Hatef, Ali; Sadeghi, Seyed M; Fortin-Deschênes, Simon; Boulais, Etienne; Meunier, Michel

    2013-03-11

    It is well-known that optical properties of semiconductor quantum dots can be controlled using optical cavities or near fields of localized surface plasmon resonances (LSPRs) of metallic nanoparticles. In this paper we study the optics, energy transfer pathways, and exciton states of quantum dots when they are influenced by the near fields associated with plasmonic meta-resonances. Such resonances are formed via coherent coupling of excitons and LSPRs when the quantum dots are close to metallic nanorods and driven by a laser beam. Our results suggest an unprecedented sensitivity to the refractive index of the environment, causing significant spectral changes in the Förster resonance energy transfer from the quantum dots to the nanorods and in exciton transition energies. We demonstrate that when a quantum dot-metallic nanorod system is close to its plasmonic meta-resonance, we can adjust the refractive index to: (i) control the frequency range where the energy transfer from the quantum dot to the metallic nanorod is inhibited, (ii) manipulate the exciton transition energy shift of the quantum dot, and (iii) disengage the quantum dot from the metallic nanoparticle and laser field. Our results show that near meta-resonances the spectral forms of energy transfer and exciton energy shifts are strongly correlated to each other.

  3. Effects of excitation spectral width on decay profile of weakly confined excitons

    International Nuclear Information System (INIS)

    Kojima, O.; Isu, T.; Ishi-Hayase, J.; Kanno, A.; Katouf, R.; Sasaki, M.; Tsuchiya, M.

    2008-01-01

    We report the effect due to a simultaneous excitation of several exciton states on the radiative decay profiles on the basis of the nonlocal response of weakly confined excitons in GaAs thin films. In the case of excitation of single exciton state, the transient grating signal has two decay components. The fast decay component comes from nonlocal response, and the long-lived component is attributed to free exciton decay. With an increase of excitation spectral width, the nonlocal component becomes small in comparison with the long-lived component, and disappears under irradiation of a femtosecond-pulse laser with broader spectral width. The transient grating spectra clearly indicates the contribution of the weakly confined excitons to the signal, and the exciton line width hardly changes by excitation spectral width. From these results, we concluded that the change of decay profile is attributed not to the many-body effect but to the effect of simultaneous excitation of several exciton states

  4. Highly mobile charge-transfer excitons in two-dimensional WS2/tetracene heterostructures

    Science.gov (United States)

    Zhu, Tong; Yuan, Long; Zhao, Yan; Zhou, Mingwei; Wan, Yan; Mei, Jianguo; Huang, Libai

    2018-01-01

    Charge-transfer (CT) excitons at heterointerfaces play a critical role in light to electricity conversion using organic and nanostructured materials. However, how CT excitons migrate at these interfaces is poorly understood. We investigate the formation and transport of CT excitons in two-dimensional WS2/tetracene van der Waals heterostructures. Electron and hole transfer occurs on the time scale of a few picoseconds, and emission of interlayer CT excitons with a binding energy of ~0.3 eV has been observed. Transport of the CT excitons is directly measured by transient absorption microscopy, revealing coexistence of delocalized and localized states. Trapping-detrapping dynamics between the delocalized and localized states leads to stretched-exponential photoluminescence decay with an average lifetime of ~2 ns. The delocalized CT excitons are remarkably mobile with a diffusion constant of ~1 cm2 s−1. These highly mobile CT excitons could have important implications in achieving efficient charge separation. PMID:29340303

  5. Exciton luminescence in CdxMn1-xTe compounds

    International Nuclear Information System (INIS)

    Caraman, M.; Gashin, P.; Metelitsa, Snejana; Nicorici, Valentina; Nicorici, A.

    2002-01-01

    The Cd x Mn 1-x Te (0.5 7 W/cm 2 . The luminescence spectra were observed at 78 K. The results of the study had shown that the presence of relatively narrow luminescence peaks localized in the region of the fundamental absorption edge is characteristic for these spectra and for the majority of the crystals a wide maximum in the long wavelength region is observed. The luminescence maxima with an accuracy of ∼ 5 meV correspond to the resonance energy of the excitons of the state with n=1 determined from the absorption spectra. Hence, these maxima can be considered as exciton luminescence stimulated either by the excitons of the state n=1 or bounded to the exciton ionization centers. From the analysis of the absorption and exciton luminescence spectra one can make a conclusion about the fact that the homogeneity extent of the crystals decreases from CdTe to the compounds with x= 0.8 - 0.7 and slightly increases at the x decrease to 0.5. The exciton luminescence lines in CdTe and Cd 0.99 Mn 0.01 Te crystals is shifting by 7 - 10 meV relatively to the lines of free excitons absorption. This fact is explained by the fact that in these crystals, probably, excitons bounding to the lattice inherited defects with the binding energy of 7 - 10 meV participate in the luminescence. In the long wavelength region a wide peak is observed on which the impurity lines are not displayed. In the luminescence spectra of CdTe with 0.1%. As crystals three maxima at 1.51 eV, 1.46 eV and 1.42 eV are revealed. For pure CdTe the maximum at 1.4 eV is also revealed. These maxima are explained by the luminescence through the recombination levels localized at 0.46 eV. (authors)

  6. Semiconductor nanoparticles with spatial separation of charge carriers: synthesis and optical properties

    International Nuclear Information System (INIS)

    Vasiliev, Roman B; Dirin, Dmitry N; Gaskov, Alexander M

    2011-01-01

    The results of studies on core/shell semiconductor nanoparticles with spatial separation of photoexcited charge carriers are analyzed and generalized. Peculiarities of the electronic properties of semiconductor/semiconductor heterojunctions formed inside such particles are considered. Data on the effect of spatial separation of charge carriers on the optical properties of nanoparticles including spectral shifts of the exciton bands, absorption coefficients and electron–hole pair recombination times are presented. Methods of synthesis of core/shell semiconductor nanoparticles in solutions are discussed. Specific features of the optical properties of anisotropic semiconductor nanoparticles with the semiconductor/semiconductor junctions are noted. The bibliography includes 165 references.

  7. Engineering and manipulating exciton wave packets

    Science.gov (United States)

    Zang, Xiaoning; Montangero, Simone; Carr, Lincoln D.; Lusk, Mark T.

    2017-05-01

    When a semiconductor absorbs light, the resulting electron-hole superposition amounts to a uncontrolled quantum ripple that eventually degenerates into diffusion. If the conformation of these excitonic superpositions could be engineered, though, they would constitute a new means of transporting information and energy. We show that properly designed laser pulses can be used to create such excitonic wave packets. They can be formed with a prescribed speed, direction, and spectral make-up that allows them to be selectively passed, rejected, or even dissociated using superlattices. Their coherence also provides a handle for manipulation using active, external controls. Energy and information can be conveniently processed and subsequently removed at a distant site by reversing the original procedure to produce a stimulated emission. The ability to create, manage, and remove structured excitons comprises the foundation for optoexcitonic circuits with application to a wide range of quantum information, energy, and light-flow technologies. The paradigm is demonstrated using both tight-binding and time-domain density functional theory simulations.

  8. Exciton dephasing and biexciton binding in CdSe/ZnSe islands

    DEFF Research Database (Denmark)

    Wagner, Hans Peter; Tranitz, H.-P.; Preis, H

    1999-01-01

    The dephasing of excitons and the formation of biexcitons in self-organized CdSe/ZnSe islands grown by molecular-beam epitaxy is investigated using spectrally resolved four-wave mixing. A distribution of exciton-exciton scattering efficiencies and dephasing times in the range of 0.5-10 ps...

  9. Excitonic magnetism in d.sup.6./sup. perovskites

    Czech Academy of Sciences Publication Activity Database

    Afonso, J.F.; Kuneš, Jan

    2017-01-01

    Roč. 95, č. 11 (2017), s. 1-8, č. článku 115131. ISSN 2469-9950 EU Projects: European Commission(XE) 646807 - EXMAG Institutional support: RVO:68378271 Keywords : excitonic magnetism * cobaltites Subject RIV: BM - Solid Matter Physics ; Magnetism OBOR OECD: Condensed matter physics (including formerly solid state physics, supercond.) Impact factor: 3.836, year: 2016

  10. Synthesis and Exciton Dynamics of Triplet Sensitized Conjugated Polymers

    KAUST Repository

    Andernach, Rolf; Utzat, Hendrik; Dimitrov, Stoichko; McCulloch, Iain; Heeney, Martin; Durrant, James; Bronstein, Hugo

    2015-01-01

    We report the synthesis of a novel polythiophene-based host-guest copolymer incorporating a Pt-porphyrin complex (TTP-Pt) into the backbone for efficient singlet to triplet polymer exciton sensitization. We elucidated the exciton dynamics in thin

  11. The creation of defects in ammonium halides by excitons

    International Nuclear Information System (INIS)

    Kim, L.M.

    2002-01-01

    The ammonium halides crystals and alkali halides crystals are analogous by kind chemical bonds and crystalline lattices. The anionic sublattice is identical in this crystals. It is known the main mechanism of defect creation by irradiation is radiationless decay of excitons in alkali halides crystals. The F-, H-centers are formation in this processes. However, F, H-centres are not detected in ammonium halides. The goal of this work is investigation the creation of defects in ammonium halides by excitons. We established that excitons in ammonium chlorides and bromides are similar to excitons in alkali halides. It is known excitons are self-trapped and have identical parameters of the exciton-phonon interaction in both kind crystals. It is supposed, that processes of radiationless disintegration of excitons are identical in ammonium and alkali halides. It is necessary to understand why F-, H-centers are absent in ammonium halides. V k -centres are created by the excitation of the ammonium halides crystals in the absorption band of excitons. It was established by thermoluminescence and spectrums of absorption. The V k -centers begin to migrate at 110-120 K in ammonium chlorides and bromides. The curve of thermoluminescence have peak with maximum at this temperatures. It is known V k -centers in ammonium chlorides have the absorption band at 380 nm. We discovered this absorption band after irradiation of crystals by ultra-violet. In alkali halides F-center is anionic vacancy with electron. The wave function of electron are spread ed at the cations around anionic vacancy. We established the cation NH 4 + in ammonium halides can to capture electron. The ion NH 4 2+ is unsteady. It is disintegrated to NH 3 + and H + . We suppose that excitons in ammonium and alkali halides are disintegrated identically. When cation NH 4 + capture electron, in the anionic sublattice the configuration are created in a direction (100) The indicated configuration is unsteady in relation to a

  12. Bose-Einstein condensation of excitons in Cu2O

    International Nuclear Information System (INIS)

    Snoke, D.W.

    1990-01-01

    Free excitons provide the only experimental system other than helium in which the behavior of particles with mass is known to follow Bose-Einstein statistics. Experimental observations are presented of the kinetic energy distribution of excitons in the direct-gap semiconductor Cu 2 O, both the triplet orthoexciton state and the singlet paraexciton state. The density and temperature of the exciton gas closely follow the phase boundary for Bose-Einstein condensation. At the highest densities, the lower-lying paraexcitons take on an anomalous energy distribution with a sharp, high-energy edge. This odd distribution of particle energies may be associated with Bose-Einstein condensation into a state with nonzero momentum. Indeed, the excitons leave the region of their creation at supersonic velocities. In addition to the experimental observations, theoretical models are presented for several aspects of this nonequilibrium system. The equilibration of a nearly-ideal boson gas is modeled, finding that a significant time is required for the approach to condensation. The temperature and density of the excitons in steady state are modeled based on known classical kinetic effects in semiconductors, and the effects of Bose-Einstein statistics on these processes estimated

  13. Some evidence for the high density phase of excitons in CdS

    International Nuclear Information System (INIS)

    Rueckmann, I.; May, V.; Voigt, J.

    1980-01-01

    Reflection spectra without and with additional pumping are measured in CdS at 1.8 and 77 K, respectively, starting from very low pump intensities. At low pump intensities a special behaviour of the reflection minimum is found indicating the importance of an exciton dead layer. The experimental spectra up to the highest pump intensities can be fitted very well taking into account spatial dispersion, exciton dead layer, and density dependent excitonic parameters. Polarizability, damping, and layer thickness change continuously in the whole range of excitation intensities. On the other side, the transverse dielectric function of a high density gas of interacting 1s excitons is calculated. A comparison between theoretically and experimentally obtained excitonic parameters at different densities shows good agreement. Hence, the importance of many-exciton interaction for the reflection spectra up to vanishing at highest pump intensities is concluded. (author)

  14. Self-trapped excitons in LH2 bacteriochlorophyll-protein complexes under high pressure

    International Nuclear Information System (INIS)

    Timpmann, K.; Ellervee, Aleksandr; Kuznetsov, Anatoli; Laisaar, Arlentin; Trinkunas, Gediminas; Freiberg, Arvi

    2003-01-01

    The absorption and emission spectra of excitons in LH2 antenna complexes from the photosynthetic purple bacterium Rhodobacter sphaeroides have been studied under hydrostatic pressure. The measurements made between ambient pressure and 6 kbar over a broad temperature range reveal largely different rates of the pressure-induced shifts for the absorption and emission bands. Numerical calculations based on exciton polaron model provide evidence for the exciton self-trapping at ambient pressure as well as for the pressure stabilization of the self-trapped exciton states responsible for the emission, whereas the light absorbing states belong to nearly free excitons over the whole pressure and temperature ranges studied

  15. Excitonic and Polaronic Properties of 2D Hybrid Organic–Inorganic Perovskites

    KAUST Repository

    Yin, Jun; Li, Hong; Cortecchia, Daniele; Soci, Cesare; Bredas, Jean-Luc

    2017-01-01

    calculations including corrections due to spin orbit couplings and electron hole interactions, a computationally intensive molecular cluster approach is exploited to describe the excitonic and polaronic properties of these 2D perovskites at the atomistic level

  16. Phonon-assisted two-photon exciton transitions in semiconductors

    International Nuclear Information System (INIS)

    Hassan, A.R.

    1987-08-01

    The theory of phonon-assisted two-photon transitions to excitonic states in semiconductors has been theoretically investigated. The effects of both the nonparabolicity of the band and the degeneracy of the valence band have been taken into account. Expressions for the absorption coefficient through different band models are calculated. The numerical applications to CdI 2 and GaP show that the 4-band model gives the dominant contribution which leads to a final s-exciton state. An exciton peak appears at an energy which is close to that recently observed in CdI 2 . The non-parabolic effect enhances the absorption coefficient by a two-order of magnitude. (author). 6 refs, 1 fig., 1 tab

  17. 4P-NPD ultra-thin films as efficient exciton blocking layers in DBP/C70 based organic solar cells

    Science.gov (United States)

    Patil, Bhushan R.; Liu, Yiming; Qamar, Talha; Rubahn, Horst-Günter; Madsen, Morten

    2017-09-01

    Exciton blocking effects from ultra-thin layers of N,N‧-di-1-naphthalenyl-N,N‧-diphenyl [1,1‧:4‧,1″:4″,1‴-quaterphenyl]-4,4‴-diamine (4P-NPD) were investigated in small molecule-based inverted organic solar cells (OSCs) using tetraphenyldibenzoperiflanthene as the electron donor material and fullerene (C70) as the electron acceptor material. The short-circuit current density (J SC) and power conversion efficiency (PCE) of the optimized OSCs with 0.7 nm thick 4P-NPD were approximately 16% and 24% higher, respectively, compared to reference devices without exciton blocking layers (EBLs). Drift diffusion-based device modeling was conducted to model the full current density-voltage (JV) characteristics and external quantum efficiency spectrum of the OSCs, and photoluminescence measurements were conducted to investigate the exciton blocking effects with increasing thicknesses of the 4P-NPD layer. Importantly, coupled optical and electrical modeling studies of the device behaviors and exciton generation rates and densities in the active layer for different 4P-NPD layer thicknesses were conducted, in order to gain a complete understanding of the observed increase in PCE for 4P-NPD layer thicknesses up to 1 nm, and the observed decrease in PCE for layer thicknesses beyond 1 nm. This work demonstrates a route for guiding the integration of EBLs in OSC devices.

  18. Exciton-polaron quenching in organic thin-film transistors studied by fluorescence lifetime imaging microscopy

    DEFF Research Database (Denmark)

    Jensen, Per Baunegaard With; Leißner, Till; Osadnik, Andreas

    Organic semiconductors show great potential in electronic and optical applications. However, a major challenge is the degradation of the semiconductor materials that cause a reduction in device performance. Here, we present our investigations of Organic Thin Film Transistors (OTFT) based...... that correlates with the local charge density indicates a pronounced exciton quenching by the injected charges. Subsequent FLIM measurements on previously biased OTFT devices show a general decrease in fluorescence lifetime suggesting degradation of the organic semiconductor. This is correlated with the results...

  19. Exciton diffusion coefficient measurement in ZnO nanowires under electron beam irradiation

    Science.gov (United States)

    Donatini, Fabrice; Pernot, Julien

    2018-03-01

    In semiconductor nanowires (NWs) the exciton diffusion coefficient can be determined using a scanning electron microscope fitted with a cathodoluminescence system. High spatial and temporal resolution cathodoluminescence experiments are needed to measure independently the exciton diffusion length and lifetime in single NWs. However, both diffusion length and lifetime can be affected by the electron beam bombardment during observation and measurement. Thus, in this work the exciton lifetime in a ZnO NW is measured versus the electron beam dose (EBD) via a time-resolved cathodoluminescence experiment with a temporal resolution of 50 ps. The behavior of the measured exciton lifetime is consistent with our recent work on the EBD dependence of the exciton diffusion length in similar NWs investigated under comparable SEM conditions. Combining the two results, the exciton diffusion coefficient in ZnO is determined at room temperature and is found constant over the full span of EBD.

  20. Charge separation in excitonic and bipolar solar cells - A detailed balance approach

    International Nuclear Information System (INIS)

    Kirchartz, Thomas; Rau, Uwe

    2008-01-01

    A generalized solar cell model for excitonic and classical, bipolar solar cells is developed that describes the combined transport and interaction of electrons, holes and excitons. Both, conventional inorganic solar cells as well as organic solar cells, where excitons play a dominant role for energy transport, turn out to be special cases of this model. Due to the inclusion of photon recycling effects, the approach is compatible with the principle of detailed balance and the Shockley-Queisser limit. We show how varying the interaction between excitons and charge carriers as well as varying the respective mobilities of the different species changes the operation mode of the solar cell path between excitonic and bipolar

  1. A study of polaritonic transparency in couplers made from excitonic materials

    Energy Technology Data Exchange (ETDEWEB)

    Singh, Mahi R.; Racknor, Chris [Department of Physics and Astronomy, Western University, London, Ontario N6A 3K7 (Canada)

    2015-03-14

    We have studied light matter interaction in quantum dot and exciton-polaritonic coupler hybrid systems. The coupler is made by embedding two slabs of an excitonic material (CdS) into a host excitonic material (ZnO). An ensemble of non-interacting quantum dots is doped in the coupler. The bound exciton polariton states are calculated in the coupler using the transfer matrix method in the presence of the coupling between the external light (photons) and excitons. These bound exciton-polaritons interact with the excitons present in the quantum dots and the coupler is acting as a reservoir. The Schrödinger equation method has been used to calculate the absorption coefficient in quantum dots. It is found that when the distance between two slabs (CdS) is greater than decay length of evanescent waves the absorption spectrum has two peaks and one minimum. The minimum corresponds to a transparent state in the system. However, when the distance between the slabs is smaller than the decay length of evanescent waves, the absorption spectra has three peaks and two transparent states. In other words, one transparent state can be switched to two transparent states when the distance between the two layers is modified. This could be achieved by applying stress and strain fields. It is also found that transparent states can be switched on and off by applying an external control laser field.

  2. Plasmon exciton-polariton lasing

    NARCIS (Netherlands)

    Ramezani, M.; Halpin, H.A.; Feist, J.; Fernández-Dominguez, A.; Rodriguez, S.R.K.; Garcia-Vidal, F.J.; Gomez-Rivas, J.

    2017-01-01

    Strong light-matter interaction leads to the appearance of new states, i.e. exciton-polaritons, with photophysical properties rather distinct from their constituents. Recent developments in fabrication techniques allow us to make metallic structures with strong electric field confinement in

  3. Two exciton states in discrete and continuum alpha-helical proteins

    International Nuclear Information System (INIS)

    Latha, M.M.; Merlin, G.

    2012-01-01

    The dynamics of alpha-helical proteins is described by proposing a model Hamiltonian representing two exciton bound states. The dynamics is studied by constructing the equations of motion using a two exciton eigen-function in the discrete level. A numerical analysis shows the existence of two excitons in alpha-helical proteins and its propagation as solitons along the hydrogen bonding spines. The lattice model is also treated in the continuum limit which is a valid approximation in the low temperature, long wavelength limit. The resulting equation is studied using the multiple scale perturbation analysis which also shows the transfer of two exciton energy through alpha-helical proteins in the form of solitons with no change in velocity and amplitude. -- Highlights: ► The dynamics of alpha-helical proteins with two exciton states is studied. ► The dynamics is studied both in the discrete and continuum levels. ► The resulting equations are solved numerically and analytically. ► The solution supports the propagation of the energy in the form of solitons.

  4. Detuning-Controlled Internal Oscillations in an Exciton-Polariton Condensate

    Science.gov (United States)

    Voronova, N. S.; Elistratov, A. A.; Lozovik, Yu. E.

    2015-10-01

    We theoretically analyze exciton-photon oscillatory dynamics within a homogenous polariton gas in the presence of energy detuning between the cavity and quantum well modes. Whereas pure Rabi oscillations consist of the particle exchange between the photon and exciton states in the polariton system without any oscillations of the phases of the two subcondensates, we demonstrate that any nonzero detuning results in oscillations of the relative phase of the photon and exciton macroscopic wave functions. Different initial conditions reveal a variety of behaviors of the relative phase between the two condensates, and a crossover from Rabi-like to Josephson-like oscillations is predicted.

  5. 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.

  6. Coherent dynamics of excitons in a stack of self-assembled InAs quantum dots at 1.5-μm waveband

    International Nuclear Information System (INIS)

    Ishi-Hayase, J.; Akahane, K.; Yamamoto, N.; Kujiraoka, M.; Inoue, J.; Ema, K.; Tsuchiya, M.; Sasaki, M.

    2006-01-01

    We investigate the excitonic dephasing in a stack of self-assembled quantum dots (SAQDs) by using a four-wave-mixing (FWM) technique performed in the optical telecomm-fiber wavelength region at 6 K. A sample used in our experiment is a 150-layer stack of InAs SAQDs embedded in InGaAlAs grown on InP(3 1 1)B substrate fabricated by molecular beam epitaxy. By using a novel strain-controlled technique, the resonant wavelength of the exciton ground state (GS) ranges from 1.25 to 1.5 μm which is much longer than that in typical In(Ga)As SAQDs. In the weak excitation region, the intrinsic dephasing time of excitons at the excitation wavelength of 1.43 μm reaches 770 ps which is much longer than that in most SAQDs with the resonant wavelength of <1 μm. We also find a strong anisotoropy of the signal intensity with respect to the crystal axis attributed to the orientation of InP(3 1 1)B substrate and the elongated shape of QDs

  7. Delocalization of Coherent Triplet Excitons in Linear Rigid Rod Conjugated Oligomers.

    Science.gov (United States)

    Hintze, Christian; Korf, Patrick; Degen, Frank; Schütze, Friederike; Mecking, Stefan; Steiner, Ulrich E; Drescher, Malte

    2017-02-02

    In this work, the triplet state delocalization in a series of monodisperse oligo(p-phenyleneethynylene)s (OPEs) is studied by pulsed electron paramagnetic resonance (EPR) and pulsed electron nuclear double resonance (ENDOR) determining zero-field splitting, optical spin polarization, and proton hyperfine couplings. Neither the zero-field splitting parameters nor the optical spin polarization change significantly with OPE chain length, in contrast to the hyperfine coupling constants, which showed a systematic decrease with chain length n according to a 2/(1 + n) decay law. The results provide striking evidence for the Frenkel-type nature of the triplet excitons exhibiting full coherent delocalization in the OPEs under investigation with up to five OPE repeat units and with a spin density distribution described by a nodeless particle in the box wave function. The same model is successfully applied to recently published data on π-conjugated porphyrin oligomers.

  8. Bose Condensation of Interwell Excitons in Double Quantum Wells

    DEFF Research Database (Denmark)

    Larionov, A. V.; Timofeev, V. B.; Ni, P. A.

    2002-01-01

    The luminescence of interwell excitons in double quantum wells GaAs/AlGaAs (n–i–n heterostructures) with large-scale fluctuations of random potential in the heteroboundary planes was studied. The properties of excitons whose photoexcited electron and hole are spatially separated in the neighboring...

  9. Photogenerated Exciton Dissociation in Highly Coupled Lead Salt Nanocrystal Assemblies

    KAUST Repository

    Choi, Joshua J.; Luria, Justin; Hyun, Byung-Ryool; Bartnik, Adam C.; Sun, Liangfeng; Lim, Yee-Fun; Marohn, John A.; Wise, Frank W.; Hanrath, Tobias

    2010-01-01

    Internanocrystal coupling induced excitons dissociation in lead salt nanocrystal assemblies is investigated. By combining transient photoluminescence spectroscopy, grazing incidence small-angle X-ray scattering, and time-resolved electric force microscopy, we show that excitons can dissociate, without the aid of an external bias or chemical potential gradient, via tunneling through a potential barrier when the coupling energy is comparable to the exciton binding energy. Our results have important implications for the design of nanocrystal-based optoelectronic devices. © 2010 American Chemical Society.

  10. Photogenerated Exciton Dissociation in Highly Coupled Lead Salt Nanocrystal Assemblies

    KAUST Repository

    Choi, Joshua J.

    2010-05-12

    Internanocrystal coupling induced excitons dissociation in lead salt nanocrystal assemblies is investigated. By combining transient photoluminescence spectroscopy, grazing incidence small-angle X-ray scattering, and time-resolved electric force microscopy, we show that excitons can dissociate, without the aid of an external bias or chemical potential gradient, via tunneling through a potential barrier when the coupling energy is comparable to the exciton binding energy. Our results have important implications for the design of nanocrystal-based optoelectronic devices. © 2010 American Chemical Society.

  11. Optical properties of single-layer, double-layer, and bulk MoS2

    Energy Technology Data Exchange (ETDEWEB)

    Molina-Sanchez, Alejandro; Wirtz, Ludger [University of Luxembourg (Luxembourg); Hummer, Kerstin [University of Vienna, Vienna (Austria)

    2013-07-01

    The rise of graphene has brought attention also to other layered materials that can complement graphene or that can be an alternative in applications as transistors. Single-layer MoS{sub 2} has shown interesting electronic and optical properties such as as high electron mobility at room temperature and an optical bandgap of 1.8 eV. This makes the material suitable for transistors or optoelectronic devices. We present a theoretical study of the optical absorption and photoluminescence spectra of single-layer, double-layer and bulk MoS{sub 2}. The excitonic states have been calculated in the framework of the Bethe-Salpeter equation, taking into account the electron-hole interaction via the screened Coulomb potential. In addition to the step-function like behaviour that is typical for the joint-density of states of 2D materials with parabolic band dispersion, we find a bound excitonic peak that is dominating the luminescence spectra. The peak is split due to spin-orbit coupling for the single-layer and split due to layer-layer interaction for few-layer and bulk MoS{sub 2}. We discuss the changes of the optical bandgap and of the exciton binding energy with the number of layers, comparing our results with the reported experimental data.

  12. Final Report, DOE grant DE-FG02-99ER45780, "Indirect Excitons in Coupled Quantum Wells"

    Energy Technology Data Exchange (ETDEWEB)

    Snoke, david W. [University of Pittsburgh

    2014-07-21

    The is the final technical report for this project, which was funded by the DOE from 1999 to 2012. The project focused on experimental studies of spatially indirect excitons in coupled quantum wells, with the aim of understanding the quantum physics of these particles, including such effects as pattern formation due to electron-hole charge separation, the Mott plasma-insulator transition, luminescence up-conversion through field-assisted tunneling, luminescence line shifts due to many-body renormalization and magnetic field effects on tunneling, and proposed effects such as Bose-Einstein condensation of indirect excitons and phase separation of bright and dark indirect excitons. Significant results are summarized here and the relation to other work is discussed.

  13. Optical properties of alkali halide crystals from all-electron hybrid TD-DFT calculations

    Energy Technology Data Exchange (ETDEWEB)

    Webster, R., E-mail: ross.webster07@imperial.ac.uk; Harrison, N. M. [Thomas Young Centre, Department of Chemistry, Imperial College London, South Kensington, London SW7 2AZ (United Kingdom); Bernasconi, L. [Rutherford Appleton Laboratory, STFC, Harwell Oxford, Didcot OX11 0QX (United Kingdom)

    2015-06-07

    We present a study of the electronic and optical properties of a series of alkali halide crystals AX, with A = Li, Na, K, Rb and X = F, Cl, Br based on a recent implementation of hybrid-exchange time-dependent density functional theory (TD-DFT) (TD-B3LYP) in the all-electron Gaussian basis set code CRYSTAL. We examine, in particular, the impact of basis set size and quality on the prediction of the optical gap and exciton binding energy. The formation of bound excitons by photoexcitation is observed in all the studied systems and this is shown to be correlated to specific features of the Hartree-Fock exchange component of the TD-DFT response kernel. All computed optical gaps and exciton binding energies are however markedly below estimated experimental and, where available, 2-particle Green’s function (GW-Bethe-Salpeter equation, GW-BSE) values. We attribute this reduced exciton binding to the incorrect asymptotics of the B3LYP exchange correlation ground state functional and of the TD-B3LYP response kernel, which lead to a large underestimation of the Coulomb interaction between the excited electron and hole wavefunctions. Considering LiF as an example, we correlate the asymptotic behaviour of the TD-B3LYP kernel to the fraction of Fock exchange admixed in the ground state functional c{sub HF} and show that there exists one value of c{sub HF} (∼0.32) that reproduces at least semi-quantitatively the optical gap of this material.

  14. Vacuum ultraviolet synchrotron measurements of excitons in NaMgF{sub 3}:Yb{sup 2+}

    Energy Technology Data Exchange (ETDEWEB)

    Hughes-Currie, Rosa B. [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); Ivanovskikh, Konstantin V. [ANK Service Ltd., PB 58, Novouralsk 624131, Sverdlovsk Region (Russian Federation); Ural Federal University, 19 Mira st., Ekaterinburg 620002 (Russian Federation); Reid, Michael F., E-mail: mike.reid@canterbury.ac.nz [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); MacDiarmid Institute for Advanced Materials and Nanotechnology (New Zealand); Wells, Jon-Paul R. [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); Dodd-Walls Centre for Quantum and Photonic Technologies (New Zealand); Reeves, Roger J. [Department of Physics and Astronomy, University of Canterbury, PB 4800, Christchurch 8140 (New Zealand); MacDiarmid Institute for Advanced Materials and Nanotechnology (New Zealand); Meijerink, Andries [Debye Institute, Utrecht University, P.O. Box 80 000, 3508 TA Utrecht (Netherlands)

    2016-01-15

    Results of a vacuum ultraviolet spectroscopic characterization of NaMgF{sub 3}:Yb{sup 2+} are presented. The material demonstrates emission features associated with self-trapped excitons and impurity-trapped excitons. The emission features noticeably overlap giving rise to a broad emission band from 17 000 to 35 000 cm{sup −1} at a sample temperature of 8 K. To identify the true profiles of the emission features we have used a deconvolution procedure. The deconvolution was possible due to the thermal quenching of self-trapped excitons at room temperature that allowed for direct observations of the impurity trapped exciton emission band. Energy transfer between host electronic excitations (excitons and e–h pairs) and Yb{sup 2+} ions leading to the formation of impurity-trapped excitons is evident from excitation spectra. - Highlights: • We present VUV emission and excitation spectra of NaMgF{sub 3}:Yb{sup 2+}. • Formation of free excitons leads to emission from intrinsic and extrinsic excitons. • We deconvolute the emission to separate the two overlapping exciton bands. • The excitation spectra show two mechanisms for forming impurity-trapped excitons.

  15. Structural tunability and switchable exciton emission in inorganic-organic hybrids with mixed halides

    Science.gov (United States)

    Ahmad, Shahab; Baumberg, Jeremy J.; Vijaya Prakash, G.

    2013-12-01

    Room-temperature tunable excitonic photoluminescence is demonstrated in alloy-tuned layered Inorganic-Organic (IO) hybrids, (C12H25NH3)2PbI4(1-y)Br4y (y = 0 to 1). These perovskite IO hybrids adopt structures with alternating stacks of low-dimensional inorganic and organic layers, considered to be naturally self-assembled multiple quantum wells. These systems resemble stacked monolayer 2D semiconductors since no interlayer coupling exists. Thin films of IO hybrids exhibit sharp and strong photoluminescence (PL) at room-temperature due to stable excitons formed within the low-dimensional inorganic layers. Systematic variation in the observed exciton PL from 510 nm to 350 nm as the alloy composition is changed, is attributed to the structural readjustment of crystal packing upon increase of the Br content in the Pb-I inorganic network. The energy separation between exciton absorption and PL is attributed to the modified exciton density of states and diffusion of excitons from relatively higher energy states corresponding to bromine rich sites towards the lower energy iodine sites. Apart from compositional fluctuations, these excitons show remarkable reversible flips at temperature-induced phase transitions. All the results are successfully correlated with thermal and structural studies. Such structural engineering flexibility in these hybrids allows selective tuning of desirable exciton properties within suitable operating temperature ranges. Such wide-range PL tunability and reversible exciton switching in these novel IO hybrids paves the way to potential applications in new generation of optoelectronic devices.

  16. Atomistic tight-binding theory of excitonic splitting energies in CdX(X = Se, S and Te)/ZnS core/shell nanocrystals

    Science.gov (United States)

    Sukkabot, Worasak; Pinsook, Udomsilp

    2017-01-01

    Using the atomistic tight-binding theory (TB) and a configuration interaction description (CI), we numerically compute the excitonic splitting of CdX(X = Se, S and Te)/ZnS core/shell nanocrystals with the objective to explain how types of the core materials and growth shell thickness can provide the detailed manipulation of the dark-dark (DD), dark-bright (DB) and bright-bright (BB) excitonic splitting, beneficial for the active application of quantum information. To analyze the splitting of the excitonic states, the optical band gaps, ground-state wave function overlaps and atomistic electron-hole interactions tend to be numerically demonstrated. Based on the atomistic computations, the single-particle and excitonic gaps are mainly reduced with the increasing ZnS shell thickness owing to the quantum confinement. In the range of the higher to lower energies, the order of the single-particle gaps is CdSe/ZnS, CdS/ZnS and CdTe/ZnS core/shell nanocrystals, while one of the excitonic gaps is CdS/ZnS, CdSe/ZnS and CdTe/ZnS core/shell nanocrystals because of the atomistic electron-hole interaction. The strongest electron-hole interactions are mainly observed in CdSe/ZnS core/shell nanocrystals. In addition, the computational results underline that the energies of the dark-dark (DD), dark-bright (DB) and bright-bright (BB) excitonic splitting are generally reduced with the increasing ZnS growth shell thickness as described by the trend of the electron-hole exchange interaction. The high-to-low splitting of the excitonic states is demonstrated in CdSe/ZnS, CdTe/ZnS and CdS/ZnS core/shell nanocrystals because of the fashion in the electron-hole exchange interaction and overlaps of the electron-hole wave functions. As the resulting calculations, it is expected that CdS/ZnS core/shell nanocrystals are the best candidates to be the source of entangled photons. Finally, the comprehensive information on the excitonic splitting can enable the use of suitable core

  17. Decoherence suppression of excitons by bang-bang control

    International Nuclear Information System (INIS)

    Kishimoto, T.; Hasegawa, A.; Mitsumori, Y.; Ishi-Hayase, J.; Sasaki, M.; Minami, F.

    2007-01-01

    We report the demonstration of decoherence control of excitons on a layered compound semiconductor GaSe by using successive three femtosecond pulses, i.e., the six-wave mixing configuration. The second pulse acts as a π pulse which reverses the time evolution of non-Markovian dynamics. By changing the pulse interval conditions, we confirmed for the first time the suppression of exciton decoherence by π pulse irradiation

  18. Photoelectric emission from negative-electron-affinity diamond (111) surfaces: Exciton breakup versus conduction-band emission

    International Nuclear Information System (INIS)

    Bandis, C.; Pate, B.B.

    1995-01-01

    We have recently reported that bound electron-hole pairs (Mott-Wannier excitons) are the dominant source of photoelectron emission from specially prepared [''as-polished'' C(111)-(1x1):H] negative-electron-affinity diamond surfaces for near-band-gap excitation up to 0.5 eV above threshold [C. Bandis and B. B. Pate, Phys. Rev. Lett. 74, 777 (1995)]. It was found that photoexcited excitons transport to the surface, break up, and emit their electron. In this paper, we extend the study of exciton-derived emission to include partial yield (constant final-state) analysis as well as angular distribution measurements of the photoelectric emission. In addition, we find that exciton-derived emission does not always dominate. Photoelectric emission properties of the in situ ''rehydrogenated'' (111)-(1x1):H diamond surface are characteristically different than emission observed from the as-polished (111)-(1x1):H surface. The rehydrogenated surface has additional downward band bending as compared to the as-polished surface. In confirmation of the assignment of photoelectric yield to exciton breakup emission, we find a significant enhancement of the total electron yield when the downward band bending of the hydrogenated surface is increased. The functional form of the observed total electron yield demonstrates that, in contrast to the as-polished surface, conduction-band electrons are a significant component of the observed photoelectric yield from the in situ hydrogenated (111)-(1x1):H surface. Furthermore, electron emission characteristics of the rehydrogenated surface confirms our assignment of a Fan phonon-cascade mechanism for thermalization of excitons

  19. Energy Migration in Organic Thin Films--From Excitons to Polarons

    Science.gov (United States)

    Mullenbach, Tyler K.

    The rise of organic photovoltaic devices (OPVs) and organic light-emitting devices has generated interest in the physics governing exciton and polaron dynamics in thin films. Energy transfer has been well studied in dilute solutions, but there are emergent properties in thin films and greater complications due to complex morphologies which must be better understood. Despite the intense interest in energy transport in thin films, experimental limitations have slowed discoveries. Here, a new perspective of OPV operation is presented where photovoltage, instead of photocurrent, plays the fundamental role. By exploiting this new vantage point the first method of measuring the diffusion length (LD) of dark (non-luminescent) excitons is developed, a novel photodetector is invented, and the ability to watch exciton arrival, in real-time, at the donor-acceptor heterojunction is presented. Using an enhanced understanding of exciton migration in thin films, paradigms for enhancing LD by molecular modifications are discovered, and the first exciton gate is experimentally and theoretically demonstrated. Generation of polarons from exciton dissociation represents a second phase of energy migration in OPVs that remains understudied. Current approaches are capable of measuring the rate of charge carrier recombination only at open-circuit. To enable a better understanding of polaron dynamics in thin films, two new approaches are presented which are capable of measuring both the charge carrier recombination and transit rates at any OPV operating voltage. These techniques pave the way for a more complete understanding of charge carrier kinetics in molecular thin films.

  20. Influence of intra-pigment vibrations on dynamics of photosynthetic exciton.

    Science.gov (United States)

    Sato, Yoshihiro; Doolittle, Brian

    2014-11-14

    We have numerically investigated the effect of an underdamped intra-pigment vibrational mode on an exciton's quantum coherence and energy transfer efficiency. Our model describes a bacteriochlorophyll a pigment-protein dimer under the conditions at which photosynthetic energy transfer occurs. The dimer is modeled using a theoretical treatment of a vibronic exciton, and its dynamics are numerically analyzed using a non-Markovian and non-perturbative method. We examined the system's response to various values of the Huang-Rhys factor, site energy difference, reorganization energy, and reorganization energy difference. We found that the inclusion of the intra-pigment vibronic mode allows for long-lived oscillatory quantum coherences to occur. This excitonic coherence is robust against static site-energy disorder. The vibrational mode also promotes exciton transfer along the site-energy landscape thus improving the overall energy transfer efficiency.

  1. Influence of intra-pigment vibrations on dynamics of photosynthetic exciton

    International Nuclear Information System (INIS)

    Sato, Yoshihiro; Doolittle, Brian

    2014-01-01

    We have numerically investigated the effect of an underdamped intra-pigment vibrational mode on an exciton's quantum coherence and energy transfer efficiency. Our model describes a bacteriochlorophyll a pigment-protein dimer under the conditions at which photosynthetic energy transfer occurs. The dimer is modeled using a theoretical treatment of a vibronic exciton, and its dynamics are numerically analyzed using a non-Markovian and non-perturbative method. We examined the system's response to various values of the Huang-Rhys factor, site energy difference, reorganization energy, and reorganization energy difference. We found that the inclusion of the intra-pigment vibronic mode allows for long-lived oscillatory quantum coherences to occur. This excitonic coherence is robust against static site-energy disorder. The vibrational mode also promotes exciton transfer along the site-energy landscape thus improving the overall energy transfer efficiency

  2. Influence of intra-pigment vibrations on dynamics of photosynthetic exciton

    Energy Technology Data Exchange (ETDEWEB)

    Sato, Yoshihiro, E-mail: sato.yoshihiro77@nihon-u.ac.jp, E-mail: ysato.colby@gmail.com; Doolittle, Brian [Department of Physics and Astronomy, Colby College, Waterville, Maine 04901 (United States)

    2014-11-14

    We have numerically investigated the effect of an underdamped intra-pigment vibrational mode on an exciton's quantum coherence and energy transfer efficiency. Our model describes a bacteriochlorophyll a pigment-protein dimer under the conditions at which photosynthetic energy transfer occurs. The dimer is modeled using a theoretical treatment of a vibronic exciton, and its dynamics are numerically analyzed using a non-Markovian and non-perturbative method. We examined the system's response to various values of the Huang-Rhys factor, site energy difference, reorganization energy, and reorganization energy difference. We found that the inclusion of the intra-pigment vibronic mode allows for long-lived oscillatory quantum coherences to occur. This excitonic coherence is robust against static site-energy disorder. The vibrational mode also promotes exciton transfer along the site-energy landscape thus improving the overall energy transfer efficiency.

  3. From optics to superconductivity. Many body effects in transition metal dichalcogenides

    Energy Technology Data Exchange (ETDEWEB)

    Roesner, Malte; Schoenhoff, Gunnar; Wehling, Tim [Institute for Theoretical Physics, University of Bremen (Germany); Bremen Center for Computational Material Sciences, University of Bremen (Germany); Steinhoff, Alexander; Jahnke, Frank; Gies, Christopher [Institute for Theoretical Physics, University of Bremen (Germany); Haas, Stephan [Department of Physics and Astronomy, University of Southern California, Los Angeles, CA (United States)

    2015-07-01

    We discuss many body effects in MoS{sub 2} ranging from optical properties to the emergence superconductivity (SC) and charge density wave phases (CDW). Combining ab-initio theory and semiconductor Bloch equations we show that excited carriers cause a redshift of the excitonic ground-state absorption line, while higher excitonic lines disappear successively due to a huge Coulomb-induced band gap shrinkage of more than 500 meV and concomitant exciton binding-energy reductions. Upon strong charge doping, we observe a succession of semiconducting, metallic, SC, and CDW regimes. Both, the SC and the CDW instabilities trace back to a Kohn anomaly and related softening of Brillouin zone boundary phonons.

  4. Strong room-temperature ultraviolet to red excitons from inorganic organic-layered perovskites, (MX4 (M=Pb, Sn, Hg; X=I-, Br-)

    Science.gov (United States)

    Ahmad, Shahab; Prakash, G. Vijaya

    2014-01-01

    Many varieties of layered inorganic-organic (IO) perovskite of type (MX4 (where R: organic moiety, M: divalent metal, and X: halogen) were successfully fabricated and characterized. X-ray diffraction data suggest that these inorganic and organic structures are alternatively stacked up along c-axis, where inorganic mono layers are of extended corner-shared MX6 octahedra and organic spacers are the bi-layers of organic entities. These layered perovskites show unusual room-temperature exciton absorption and photoluminescence due to the quantum and dielectric confinement-induced enhancement in the exciton binding energies. A wide spectral range of optical exciton tunability (350 to 600 nm) was observed experimentally from systematic compositional variation in (i) divalent metal ions (M=Pb, Sn, Hg), (ii) halides (X=I and Br-), and (iii) organic moieties (R). Specific photoluminescence features are due to the structure of the extended MX42- network and the eventual electronic band structure. The compositionally dependent photoluminescence of these IO hybrids could be useful in various photonic and optoelectronic devices.

  5. Room-Temperature Exciton Lasing in Ultrathin Film of Coupled Nanocrystals

    International Nuclear Information System (INIS)

    Appavoo, Kannatassen; Xiaoze, Liu; Menon, Vinod; Sfeir, Matthew Y.

    2015-01-01

    We demonstrate exciton lasing in sub-wavelength coupled nanostructures at ultralow fluence threshold, as probed by femtosecond broadband emission and absorption spectroscopy. The complex spectrotemporal dynamics reveal for the first time an excitonic-to-electron-hole plasma lasing mechanism.

  6. Spectral and Dynamical Properties of Single Excitons, Biexcitons, and Trions in Cesium-Lead-Halide Perovskite Quantum Dots.

    Science.gov (United States)

    Makarov, Nikolay S; Guo, Shaojun; Isaienko, Oleksandr; Liu, Wenyong; Robel, István; Klimov, Victor I

    2016-04-13

    Organic-inorganic lead-halide perovskites have been the subject of recent intense interest due to their unusually strong photovoltaic performance. A new addition to the perovskite family is all-inorganic Cs-Pb-halide perovskite nanocrystals, or quantum dots, fabricated via a moderate-temperature colloidal synthesis. While being only recently introduced to the research community, these nanomaterials have already shown promise for a range of applications from color-converting phosphors and light-emitting diodes to lasers, and even room-temperature single-photon sources. Knowledge of the optical properties of perovskite quantum dots still remains vastly incomplete. Here we apply various time-resolved spectroscopic techniques to conduct a comprehensive study of spectral and dynamical characteristics of single- and multiexciton states in CsPbX3 nanocrystals with X being either Br, I, or their mixture. Specifically, we measure exciton radiative lifetimes, absorption cross-sections, and derive the degeneracies of the band-edge electron and hole states. We also characterize the rates of intraband cooling and nonradiative Auger recombination and evaluate the strength of exciton-exciton coupling. The overall conclusion of this work is that spectroscopic properties of Cs-Pb-halide quantum dots are largely similar to those of quantum dots of more traditional semiconductors such as CdSe and PbSe. At the same time, we observe some distinctions including, for example, an appreciable effect of the halide identity on radiative lifetimes, considerably shorter biexciton Auger lifetimes, and apparent deviation of their size dependence from the "universal volume scaling" previously observed for many traditional nanocrystal systems. The high efficiency of Auger decay in perovskite quantum dots is detrimental to their prospective applications in light-emitting devices and lasers. This points toward the need for the development of approaches for effective suppression of Auger

  7. Optical probe of Heisenberg-Kitaev magnetism in α -RuCl3

    Science.gov (United States)

    Sandilands, Luke J.; Sohn, C. H.; Park, H. J.; Kim, So Yeun; Kim, K. W.; Sears, Jennifer A.; Kim, Young-June; Noh, Tae Won

    2016-11-01

    We report a temperature-dependent optical spectroscopic study of the Heisenberg-Kitaev magnet α -RuCl3 . Our measurements reveal anomalies in the optical response near the magnetic ordering temperature. At higher temperatures, we observe a redistribution of spectral weight over a broad energy range that is associated with nearest-neighbor spin-spin correlations. This finding is consistent with highly frustrated magnetic interactions and in agreement with theoretical expectations for this class of material. The optical data also reveal significant electron-hole interaction effects, including a bound excitonic state. These results demonstrate a clear coupling between charge and spin degrees of freedom and provide insight into the properties of thermally disordered Heisenberg-Kitaev magnets.

  8. Exciton binding energy in GaAsBiN spherical quantum dot heterostructures

    Science.gov (United States)

    Das, Subhasis; Dhar, S.

    2017-03-01

    The ground state exciton binding energies (EBE) of heavy hole excitons in GaAs1-x-yBixNy - GaAs spherical quantum dots (QD) are calculated using a variational approach under 1s hydrogenic wavefunctions within the framework of effective mass approximation. Both the nitrogen and the bismuth content in the material are found to affect the binding energy, in particular for larger nitrogen content and lower dot radii. Calculations also show that the ground state exciton binding energies of heavy holes increase more at smaller dot sizes as compared to that for the light hole excitons.

  9. Structural tunability and switchable exciton emission in inorganic-organic hybrids with mixed halides

    International Nuclear Information System (INIS)

    Ahmad, Shahab; Vijaya Prakash, G.; Baumberg, Jeremy J.

    2013-01-01

    Room-temperature tunable excitonic photoluminescence is demonstrated in alloy-tuned layered Inorganic-Organic (IO) hybrids, (C 12 H 25 NH 3 ) 2 PbI 4(1−y) Br 4y (y = 0 to 1). These perovskite IO hybrids adopt structures with alternating stacks of low-dimensional inorganic and organic layers, considered to be naturally self-assembled multiple quantum wells. These systems resemble stacked monolayer 2D semiconductors since no interlayer coupling exists. Thin films of IO hybrids exhibit sharp and strong photoluminescence (PL) at room-temperature due to stable excitons formed within the low-dimensional inorganic layers. Systematic variation in the observed exciton PL from 510 nm to 350 nm as the alloy composition is changed, is attributed to the structural readjustment of crystal packing upon increase of the Br content in the Pb-I inorganic network. The energy separation between exciton absorption and PL is attributed to the modified exciton density of states and diffusion of excitons from relatively higher energy states corresponding to bromine rich sites towards the lower energy iodine sites. Apart from compositional fluctuations, these excitons show remarkable reversible flips at temperature-induced phase transitions. All the results are successfully correlated with thermal and structural studies. Such structural engineering flexibility in these hybrids allows selective tuning of desirable exciton properties within suitable operating temperature ranges. Such wide-range PL tunability and reversible exciton switching in these novel IO hybrids paves the way to potential applications in new generation of optoelectronic devices

  10. Sighting optics including an optical element having a first focal length and a second focal length

    Science.gov (United States)

    Crandall, David Lynn [Idaho Falls, ID

    2011-08-01

    One embodiment of sighting optics according to the teachings provided herein may include a front sight and a rear sight positioned in spaced-apart relation. The rear sight includes an optical element having a first focal length and a second focal length. The first focal length is selected so that it is about equal to a distance separating the optical element and the front sight and the second focal length is selected so that it is about equal to a target distance. The optical element thus brings into simultaneous focus, for a user, images of the front sight and the target.

  11. Exciton spectrum of surface-corrugated quantum wells: the adiabatic self-consistent approach

    International Nuclear Information System (INIS)

    Atenco A, N.; Perez R, F.; Makarov, N.M.

    2005-01-01

    A theory for calculating the relaxation frequency ν and the shift δ ω of exciton resonances in quantum wells with finite potential barriers and adiabatic surface disorder is developed. The adiabaticity implies that the correlation length R C for the well width fluctuations is much larger than the exciton radius a 0 (R C >> a 0 ). Our theory is based on the self-consistent Green's function method, and therefore takes into account the inherent action of the exciton scattering on itself. The self-consistent approach is shown to describe quantitatively the sharp exciton resonance. It also gives the qualitatively correct resonance picture for the transition to the classical limit, as well as within the domain of the classical limit itself. We present and analyze results for h h-exciton in a GaAs quantum well with Al 0.3 Ga 0.7 As barriers. It is established that the self-consistency and finite height of potential barriers significantly influence on the line-shape of exciton resonances, and make the values of ν and δ ω be quite realistic. In particular, the relaxation frequency ν for the ground-state resonance has a broad, almost symmetric maximum near the resonance frequency ω 0 , while the surface-induced resonance shift δ ω vanishes near ω 0 , and has different signs on the sides of the exciton resonance. (Author) 43 refs., 4 figs

  12. Creation of free excitons in solid krypton investigated by time-resolved luminescence spectroscopy

    International Nuclear Information System (INIS)

    Kisand, Vambola; Kirm, Marco; Negodin, Evgeni; Sombrowski, Elke; Steeg, Barbara; Vielhauer, Sebastian; Zimmerer, Georg

    2003-01-01

    The creation and relaxation of secondary excitons in solid Kr was investigated using energy-and time-resolved luminescence spectroscopy in the vacuum ultraviolet region. The spectrally selected emission of the free exciton (FE) was used as a probe for an investigation of the different exciton creation processes. Delayed FE creation via electron-hole recombination and 'prompt' (in terms of the time-resolution of the experiment) creation of excitons were separated. The 'prompt' creation of a FE appears in the region above threshold energy E th , which is equal to the sum of the band gap energy and the free exciton energy. 'Prompt' creation of excitons above E th is ascribed to a superposition of two processes: (i) creation of the electronic polaron complex (one-step process) and (ii) inelastic scattering of photoelectrons described in the framework of the multiple-parabolic-branch band model (two-step process). In addition, the ratio spectrum of the time-integrated FE and self-trapped exciton (STE) emission was analysed. The behaviour of the ratio spectrum is a proof that electron-hole recombination leads to STE states through FE states as precursors

  13. Selectively Modulating Triplet Exciton Formation in Host Materials for Highly Efficient Blue Electrophosphorescence.

    Science.gov (United States)

    Li, Huanhuan; Bi, Ran; Chen, Ting; Yuan, Kai; Chen, Runfeng; Tao, Ye; Zhang, Hongmei; Zheng, Chao; Huang, Wei

    2016-03-23

    The concept of limiting the triplet exciton formation to fundamentally alleviate triplet-involved quenching effects is introduced to construct host materials for highly efficient and stable blue phosphorescent organic light-emitting diodes (PhOLEDs). The low triplet exciton formation is realized by small triplet exciton formation fraction and rate with high binding energy and high reorganization energy of triplet exciton. Demonstrated in two analogue molecules in conventional donor-acceptor molecule structure for bipolar charge injection and transport with nearly the same frontier orbital energy levels and triplet excited energies, the new concept host material shows significantly suppressed triplet exciton formation in the host to avoid quenching effects, leading to much improved device efficiencies and stabilities. The low-voltage-driving blue PhOLED devices exhibit maximum efficiencies of 43.7 cd A(-1) for current efficiency, 32.7 lm W(-1) for power efficiency, and 20.7% for external quantum efficiency with low roll-off and remarkable relative quenching effect reduction ratio up to 41%. Our fundamental solution for preventing quenching effects of long-lived triplet excitons provides exciting opportunities for fabricating high-performance devices using the advanced host materials with intrinsically small triplet exciton formation cross section.

  14. Spin transport dynamics of excitons in CdTe/Cd1-xMnxTe quantum wells

    International Nuclear Information System (INIS)

    Kayanuma, Kentaro; Shirado, Eiji; Debnath, Mukul C.; Souma, Izuru; Chen, Zhanghai; Oka, Yasuo

    2001-01-01

    Transport properties of spin-polarized excitons were studied in the double quantum well system composed of Cd 0.95 Mn 0.05 Te and CdTe wells. Circular polarization degrees of the time resolved exciton photoluminescence in magnetic field showed that the spin-polarized excitons diffused from the magnetic quantum well and injected to the non-magnetic quantum well by conserving their spins. The spin-polarized excitons injected into the nonmagnetic well reaches 18% of the nonmagnetic well excitons. From the circular polarization degree and the lifetime of the magnetic quantum well excitons, the spin relaxation time of the excitons in the Cd 0.95 Mn 0.05 Te well was determined as 275 - 10 ps depending on the magnetic field strength. [copyright] 2001 American Institute of Physics

  15. Optical bulk and surface waves with negative refraction

    International Nuclear Information System (INIS)

    Agranovich, V.M.; Shen, Y.R.; Baughman, R.H.; Zakhidov, A.A.

    2004-01-01

    In materials with negative refraction, the direction of wave propagation is opposite to the direction of the wave vector. Using an approach that characterizes the optical response of a medium totally by a generalized dielectric permittivity, ε-bar (ω,k-bar), we discuss the possibility of seeing negative refraction for optical waves in a number of nonmagnetic media. These include bulk waves in organic materials and in gyrotropic materials where additional exciton-polariton waves can have a negative group velocity. It is known that dispersion of surface waves can be engineered by tailoring a surface transition layer. We show how this effect can be used to obtain surface waves with negative refraction

  16. Influence of structural defects on excitonic photoluminescence of pentacene

    International Nuclear Information System (INIS)

    Piryatins'kij, Yu.P.; Kurik, M.V.

    2011-01-01

    The exciton reflection, absorption, and photoluminescence spectra for single crystals and polycrystalline films have been studied in the temperature range of 4.2-296 K. A significant influence of structural defects arising during phase transitions on the exciton spectra of pentacene has been detected. The mechanisms of photoluminescence in single crystals and crystalline films of pentacene have been considered.

  17. Anatomy of an Exciton : Vibrational Distortion and Exciton Coherence in H- and J-Aggregates

    NARCIS (Netherlands)

    Tempelaar, Roel; Stradomska, Anna; Knoester, Jasper; Spano, Frank C.

    2013-01-01

    In organic materials, coupling of electronic excitations to vibrational degrees of freedom results in polaronic excited states. Through numerical calculations, we demonstrate that the vibrational distortion field accompanying such a polaron scales as the product of the excitonic interaction field

  18. Splitting of the excitonic peak in quantum wells with interfacial roughness

    International Nuclear Information System (INIS)

    Castella, H.; Wilkins, J.W.

    1998-01-01

    Excitons in a quantum well depend on the interfacial roughness resulting from its growth. The interface is characterized by islands of size ξ separated by one monolayer steps across which the confining potential decreases by V 0 for wider wells. A natural length is the localization length ξ 0 =πℎ/√ (2MV 0 ) characterizing the minimum size island to confine an exciton. For small islands (ξ 0 ), the absorption spectrum has a single exciton peak. As the island size ξ exceeds the localization length ξ 0 , the peak gradually splits into a doublet. Generally the spectra exhibit the following features: (1) the shape is very sensitive to ξ/ξ 0 and depends only weakly on the ratio of island size to exciton radius; (2) in the small island regime ξ 0 , the asymmetric shape of the exciton peak is correctly described by a model of white-noise potential, except for the position of the peak which still depends on the correlation length of the disorder. copyright 1998 The American Physical Society

  19. Crystalline Nanoporous Frameworks: a Nanolaboratory for Probing Excitonic Device Concepts.

    Energy Technology Data Exchange (ETDEWEB)

    Allendorf, Mark D.; Azoulay, Jason; Ford, Alexandra Caroline; Foster, Michael E.; El Gabaly Marquez, Farid; Leonard, Francois Leonard; Leong-Hau, Kirsty; Stavila, Vitalie; Talin, Albert Alec; Wong, Brian M.; Brumbach, Michael T.; Van Gough, D.; Lambert, Timothy N.; Rodriguez, Mark A.; Spoerke, Erik David; Wheeler, David Roger; Deaton, Joseph C.; Centrone, Andrea; Haney, Paul; Kinney, R.; Szalai, Veronika; Yoon, Heayoung P.

    2014-09-01

    Electro-optical organic materials hold great promise for the development of high-efficiency devices based on exciton formation and dissociation, such as organic photovoltaics (OPV) and organic light-emitting devices (OLEDs). However, the external quantum efficiency (EQE) of both OPV and OLEDs must be improved to make these technologies economical. Efficiency rolloff in OLEDs and inability to control morphology at key OPV interfaces both reduce EQE. Only by creating materials that allow manipulation and control of the intimate assembly and communication between various nanoscale excitonic components can we hope to first understand and then engineer the system to allow these materials to reach their potential. The aims of this proposal are to: 1) develop a paradigm-changing platform for probing excitonic processes composed of Crystalline Nanoporous Frameworks (CNFs) infiltrated with secondary materials (such as a complimentary semiconductor); 2) use them to probe fundamental aspects of excitonic processes; and 3) create prototype OPVs and OLEDs using infiltrated CNF as active device components. These functional platforms will allow detailed control of key interactions at the nanoscale, overcoming the disorder and limited synthetic control inherent in conventional organic materials. CNFs are revolutionary inorganic-organic hybrid materials boasting unmatched synthetic flexibility that allow tuning of chemical, geometric, electrical, and light absorption/generation properties. For example, bandgap engineering is feasible and polyaromatic linkers provide tunable photon antennae; rigid 1-5 nm pores provide an oriented, intimate host for triplet emitters (to improve light emission in OLEDs) or secondary semiconducting polymers (creating a charge-separation interface in OPV). These atomically engineered, ordered structures will enable critical fundamental questions to be answered concerning charge transport, nanoscale interfaces, and exciton behavior that are inaccessible

  20. Excitons in tunnel coupled CdTe and (Cd,Mn)Te quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Terletskii, Oleg; Ryabchenko, Sergiy; Tereshchenko, Oleksandr [Institute of Physics NASU, pr. Nauki 46, 03680 Kyiv (Ukraine); Sugakov, Volodymyr; Vertsimakha, Ganna [Institute for Nuclear Research NASU, pr. Nauki 47, 03680 Kyiv (Ukraine); Karczewski, Grzegorz [Institute of Physics PAS, Al. Lotnikow 32/46, PL-02-668 Warsaw (Poland)

    2017-05-15

    The photoluminescence (PL) from structures containing Cd{sub 0.95}Mn{sub 0.05}Te and CdTe quantum wells (QWs) separated by a narrow (1.94 nm) barrier was studied. The PL lines of comparable intensities from several possible exciton states were observed simultaneously at energy distances substantially exceeding kT. This means that the energy transfer in the studied systems is slower than the radiative recombination of the confined excitons. For the CdTe QW width of about 8.7-9 nm, indirect excitons with the electron and heavy hole chiefly localized in the CdTe and Cd{sub 1-x}Mn{sub x}Te QWs, respectively, were detected in the magnetic field. These indirect excitons have PL energy of about 10-20 meV above the PL line of the direct excitons in the CdTe QW. The observation of the PL from the indirect excitons which are not the lowest excitations in the structure is a distinctive feature of the system. Photoluminescence intensity dependence on the energy and the magnetic field. (copyright 2017 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim)

  1. Exciton polaritons and their one-dimensional localization in disordered structure with quantum wells

    International Nuclear Information System (INIS)

    Kosobukin, V.A.

    2003-01-01

    The Anderson light localization theory by disordered ultrathin layers (quantum wells), uniform in lateral directions and featuring intrinsic optical resonances, is presented. A model of the layers with delta-function resonance dielectric polarization is suggested for solution of the multiple scattering problem. Allowance made for interlayer disorder, one- and two-phoron characteristics of electromagnetic transfer, i.e. average energy density and the length of the Anderson light localization were calculated in analytical form. It is shown that in disordered structure average electromagnetic field is propagated as polaritons formed due to excessive emission of excitons between the quantum wells [ru

  2. Ordered Dissipative Structures in Exciton Systems in Semiconductor Quantum Wells

    Directory of Open Access Journals (Sweden)

    Andrey A. Chernyuk

    2006-02-01

    Full Text Available A phenomenological theory of exciton condensation in conditions of inhomogeneous excitation is proposed. The theory is applied to the study of the development of an exciton luminescence ring and the ring fragmentation at macroscopical distances from the central excitation spot in coupled quantum wells. The transition between the fragmented and the continuous ring is considered. With assumption of a defect in the structure, a possibility of a localized island of the condensed phase in a fixed position is shown. Exciton density distribution is also analyzed in the case of two spatially separated spots of the laser excitation.

  3. Charging and exciton-mediated decharging of metal nanoparticles in organic semiconductor matrices

    International Nuclear Information System (INIS)

    Ligorio, Giovanni; Vittorio Nardi, Marco; Christodoulou, Christos; Florea, Ileana; Ersen, Ovidiu; Monteiro, Nicolas-Crespo; Brinkmann, Martin; Koch, Norbert

    2014-01-01

    Gold nanoparticles (Au-NPs) were deposited on the surface of n- and p-type organic semiconductors to form defined model systems for charge storage based electrically addressable memory elements. We used ultraviolet photoelectron spectroscopy to study the electronic properties and found that the Au-NPs become positively charged because of photoelectron emission, evidenced by spectral shifts to higher binding energy. Upon illumination with light that can be absorbed by the organic semiconductors, dynamic charge neutrality of the Au-NPs could be re-established through electron transfer from excitons. The light-controlled charge state of the Au-NPs could add optical addressability to memory elements

  4. Radiationless decay, fission and fusion of excitons in irradiated molecular crystals

    International Nuclear Information System (INIS)

    Klein, Gerard.

    1977-01-01

    The creation and evolution of excited states in ionizing particle tracks were investigated. The passage of high energy ionizing particles in molecular crystals results in the formation of highly excited states which energy is generally above the molecular ionization potential. The theory of non radiative transitions, which describes the transitions from the highly excited states to the lowest singlet and triplet excitons S 1 and T 1 is developed. Among these non radiative transitions, the fission of singlet excitons into two singlet or triplet excitons of lower energies is studied experimentally. These results and a kinematics study of the S 1 and T 1 excitons in ionizing particle tracks were used to get a complete description of the scintillation. These results are in good agreement with the experimental measurements on the scintillation [fr

  5. Impact ionization of excitons in electric field of GaN and quantum wells of GaN/AlGaN

    International Nuclear Information System (INIS)

    Nel'son, D.K.; Yakobson, M.A.; Kagan, V.D.; Gil, B.; Grandjean, N.; Beaumont, B.; Massier, J.; Gibart, P.

    2001-01-01

    The effect of the exciton states impact ionization in the GaN exploit films and in the GaN/AlGaN structures with quantum wells is studied. The study was carried out through the optical method, based on the exciton photoluminescence quenching by applying the electric field. It is established that in the process of the electrons relaxation by energy and pulse the scattering on the admixtures prevails over the scattering on the acoustic phonons. The average length of the hot electrons free run is evaluated. The average length of the hot electrons free run in the GaN/AlGaN wells proved to be by the value order higher than in the GaN epitaxial films, which is conditioned by decrease in the probability of the electrons scattering in the two-dimensional case [ru

  6. Modifying the electronic and optical properties of carbon nanotubes

    Science.gov (United States)

    Kinder, Jesse M.

    The intrinsic electronic and optical properties of carbon nanotubes make them promising candidates for circuit elements and LEDs in nanoscale devices. However, applied fields and interactions with the environment can modify these intrinsic properties. This dissertation is a theoretical study of perturbations to an ideal carbon nanotube. It illustrates how transport and optical properties of carbon nanotubes can be adversely affected or intentionally modified by the local environment. The dissertation is divided into three parts. Part I analyzes the effect of a transverse electric field on the single-electron energy spectrum of semiconducting carbon nanotubes. Part II analyzes the effect of the local environment on selection rules and decay pathways relevant to dark excitons. Part III is a series of 26 appendices. Two different models for a transverse electric field are introduced in Part I. The first is a uniform field perpendicular to the nanotube axis. This model suggests the field has little effect on the band gap until it exceeds a critical value that can be tuned with strain or a magnetic field. The second model is a transverse field localized to a small region along the nanotube axis. The field creates a pair of exponentially localized bound states but has no effect on the band gap for particle transport. Part II explores the physics of dark excitons in carbon nanotubes. Two model calculations illustrate the effect of the local environment on allowed optical transitions and nonradiative recombination pathways. The first model illustrates the role of inversion symmetry in the optical spectrum. Broken inversion symmetry may explain low-lying peaks in the exciton spectrum of boron nitride nanotubes and localized photoemission around impurities and interfaces in carbon nanotubes. The second model in Part II suggests that free charge carriers can mediate an efficient nonradiative decay process for dark excitons in carbon nanotubes. The appendices in Part III

  7. Exciton spectrum of surface-corrugated quantum wells: the adiabatic self-consistent approach

    Energy Technology Data Exchange (ETDEWEB)

    Atenco A, N.; Perez R, F. [lnstituto de Fisica, Universidad Autonoma de Puebla, A.P. J-48, 72570 Puebla (Mexico); Makarov, N.M. [lnstituto de Ciencias, Universidad Autonoma de Puebla, Priv. 17 Norte No 3417, Col. San Miguel Hueyotlipan, 72050 Puebla (Mexico)

    2005-07-01

    A theory for calculating the relaxation frequency {nu} and the shift {delta} {omega} of exciton resonances in quantum wells with finite potential barriers and adiabatic surface disorder is developed. The adiabaticity implies that the correlation length R{sub C} for the well width fluctuations is much larger than the exciton radius a{sub 0} (R{sub C} >> a{sub 0}). Our theory is based on the self-consistent Green's function method, and therefore takes into account the inherent action of the exciton scattering on itself. The self-consistent approach is shown to describe quantitatively the sharp exciton resonance. It also gives the qualitatively correct resonance picture for the transition to the classical limit, as well as within the domain of the classical limit itself. We present and analyze results for h h-exciton in a GaAs quantum well with Al{sub 0.3} Ga{sub 0.7}As barriers. It is established that the self-consistency and finite height of potential barriers significantly influence on the line-shape of exciton resonances, and make the values of {nu} and {delta} {omega} be quite realistic. In particular, the relaxation frequency {nu} for the ground-state resonance has a broad, almost symmetric maximum near the resonance frequency {omega}{sub 0}, while the surface-induced resonance shift {delta} {omega} vanishes near {omega}{sub 0}, and has different signs on the sides of the exciton resonance. (Author) 43 refs., 4 figs.

  8. Harmonic Quantum Coherence of Multiple Excitons in PbS/CdS Core-Shell Nanocrystals

    Science.gov (United States)

    Tahara, Hirokazu; Sakamoto, Masanori; Teranishi, Toshiharu; Kanemitsu, Yoshihiko

    2017-12-01

    The generation and recombination dynamics of multiple excitons in nanocrystals (NCs) have attracted much attention from the viewpoints of fundamental physics and device applications. However, the quantum coherence of multiple exciton states in NCs still remains unclear due to a lack of experimental support. Here, we report the first observation of harmonic dipole oscillations in PbS/CdS core-shell NCs using a phase-locked interference detection method for transient absorption. From the ultrafast coherent dynamics and excitation-photon-fluence dependence of the oscillations, we found that multiple excitons cause the harmonic dipole oscillations with ω , 2 ω , and 3 ω oscillations, even though the excitation pulse energy is set to the exciton resonance frequency, ω . This observation is closely related to the quantum coherence of multiple exciton states in NCs, providing important insights into multiple exciton generation mechanisms.

  9. Direct determination of exciton wavefunction amplitudes by the momentum-resolved photo-electron emission experiment

    Science.gov (United States)

    Ohnishi, Hiromasa; Tomita, Norikazu; Nasu, Keiichiro

    2018-03-01

    We study conceptional problems of a photo-electron emission (PEE) process from a free exciton in insulating crystals. In this PEE process, only the electron constituting the exciton is suddenly emitted out of the crystal, while the hole constituting the exciton is still left inside and forced to be recoiled back to its original valence band. This recoil on the hole is surely reflected in the spectrum of the PEE with a statistical distribution along the momentum-energy curve of the valence band. This distribution is nothing but the square of the exciton wavefunction amplitude, since it shows how the electron and the hole are originally bound together. Thus, the momentum-resolved PEE can directly determine the exciton wavefunction. These problems are clarified, taking the Γ and the saddle point excitons in GaAs, as typical examples. New PEE experiments are also suggested.

  10. Energy dissipation of free exciton polaritons in semiconducting films

    International Nuclear Information System (INIS)

    De Crescenzi, M.; Harbeke, G.; Tosatti, E.

    1978-08-01

    The effective (thickness-dependent) light absorption coefficient K(ω,d) is discussed for thin semiconducting films in the frequency range of free, spatially dispersive exciton polaritons. We find that (i) it oscillates strongly for small film thicknesses; (ii) it exhibits a slanted peak lineshape; (iii) its integrated strength also depends upon the exciton damping and extrapolates to zero for vanishing damping

  11. Rotational symmetry breaking and topological phase transition in the exciton-polariton condensate of gapped 2D Dirac material

    Science.gov (United States)

    Lee, Ki Hoon; Lee, Changhee; Jeong, Jae-Seung; Min, Hongki; Chung, Suk Bum

    For the quantum well in an optical microcavity, the interplay of the Coulomb interaction and the electron-photon coupling can lead to the emergence of bosonic quasiparticles consisting of the exciton and the cavity photon known as polariton, which can form the Bose-Einstein condensate above a threshold density. Additional physics due to the nontrivial Berry phase comes into play when the quantum well consists of the gapped Dirac material such as the transition metal dichalcogenide (TMD) MoS2 or WTe2. Specifically, in forming excitons, the electron-photon coupling from the optical selection rule due to the Berry phase competes against, rather than cooperates with, the Coulomb interaction. We find that this competition gives rise to the spontaneous breaking of the rotational symmetry in the polariton condensate and also drives topological phase transition, both novel features in polariton condensation. We also investigate the possible detection of this competition through photoluminescence. This work was supported in part by the Institute for Basic Science of Korea (IBS) under Grant IBS-R009-Y1 and by the National Research Foundation of Korea (NRF) under the Basic Science Research Program Grant No. 2015R1D1A1A01058071.

  12. Impact of the glass transition on exciton dynamics in polymer thin films

    Science.gov (United States)

    Ehrenreich, Philipp; Proepper, Daniel; Graf, Alexander; Jores, Stefan; Boris, Alexander V.; Schmidt-Mende, Lukas

    2017-11-01

    In the development of organic electronics, unlimited design possibilities of conjugated polymers offer a wide variety of mechanical and electronic properties. Thereby, it is crucially important to reveal universal physical characteristics that allow efficient and forward developments of new chemical compounds. In particular for organic solar cells, a deeper understanding of exciton dynamics in polymer films can help to improve the charge generation process further. For this purpose, poly(3-hexylthiophene) (P3HT) is commonly used as a model system, although exciton decay kinetics have found different interpretations. Using temperature-dependent time-resolved photoluminescence spectroscopy in combination with low-temperature spectroscopic ellipsometry, we can show that P3HT is indeed a model system in which excitons follow a simple diffusion/hopping model. Based on our results we can exclude the relevance of hot-exciton emission as well as a dynamic torsional relaxation upon photoexcitation on a ps time scale. Instead, we depict the glass transition temperature of polymers to strongly affect exciton dynamics.

  13. Near-infrared exciton-polaritons in strongly coupled single-walled carbon nanotube microcavities

    Science.gov (United States)

    Graf, Arko; Tropf, Laura; Zakharko, Yuriy; Zaumseil, Jana; Gather, Malte C.

    2016-10-01

    Exciton-polaritons form upon strong coupling between electronic excitations of a material and photonic states of a surrounding microcavity. In organic semiconductors the special nature of excited states leads to particularly strong coupling and facilitates condensation of exciton-polaritons at room temperature, which may lead to electrically pumped organic polariton lasers. However, charge carrier mobility and photo-stability in currently used materials is limited and exciton-polariton emission so far has been restricted to visible wavelengths. Here, we demonstrate strong light-matter coupling in the near infrared using single-walled carbon nanotubes (SWCNTs) in a polymer matrix and a planar metal-clad cavity. By exploiting the exceptional oscillator strength and sharp excitonic transition of (6,5) SWCNTs, we achieve large Rabi splitting (>110 meV), efficient polariton relaxation and narrow band emission (<15 meV). Given their high charge carrier mobility and excellent photostability, SWCNTs represent a promising new avenue towards practical exciton-polariton devices operating at telecommunication wavelengths.

  14. Coherent excitonic nonlinearity versus inhomogeneous broadening in single quantum wells

    DEFF Research Database (Denmark)

    Langbein, Wolfgang Werner; Borri, Paola; Hvam, Jørn Märcher

    1998-01-01

    The coherent response of excitons in semiconductor nanostructures, as measured in four wave mixing (FWM) experiments, depends strongly on the inhomogeneous broadening of the exciton transition. We investigate GaAs-AlGaAs single quantum wells (SQW) of 4 nm to 25 nm well width. Two main mechanisms...

  15. Effects of Organic Cation Length on Exciton Recombination in Two-Dimensional Layered Lead Iodide Hybrid Perovskite Crystals.

    Science.gov (United States)

    Gan, Lu; Li, Jing; Fang, Zhishan; He, Haiping; Ye, Zhizhen

    2017-10-19

    In recent years, 2D layered organic-inorganic lead halide perovskites have attracted considerable attention due to the distinctive quantum confinement effects as well as prominent excitonic luminescence. Herein, we show that the recombination dynamics and photoluminescence (PL) of the 2D layered perovskites can be tuned by the organic cation length. 2D lead iodide perovskite crystals with increased length of the organic chains reveal blue-shifted PL as well as enhanced relative internal quantum efficiency. Furthermore, we provide experimental evidence that the formation of face-sharing [PbI 6 ] 4- octahedron in perovskites with long alkyls induces additional confinement for the excitons, leading to 1D-like recombination. As a result, the PL spectra show enhanced inhomogeneous broadening at low temperature. Our work provides physical understanding of the role of organic cation in the optical properties of 2D layered perovskites, and would benefit the improvement of luminescence efficiency of such materials.

  16. Singlet Exciton Lifetimes in Conjugated Polymer Films for Organic Solar Cells

    KAUST Repository

    Dimitrov, Stoichko; Schroeder, Bob; Nielsen, Christian; Bronstein, Hugo; Fei, Zhuping; McCulloch, Iain; Heeney, Martin; Durrant, James

    2016-01-01

    The lifetime of singlet excitons in conjugated polymer films is a key factor taken into account during organic solar cell device optimization. It determines the singlet exciton diffusion lengths in polymer films and has a direct impact

  17. Self-localization of excitons in a periodically modulated molecular medium

    International Nuclear Information System (INIS)

    Zabolotskii, A. A.

    2006-01-01

    Electromagnetic field propagation is analyzed in a one-dimensional Bragg grating consisting of periodically arranged linear molecules making up a resonant medium. Dye J-aggregates and conjugated polymers are considered as examples of the medium. Both adiabatic and nonadiabatic dynamics of the acoustic waves generated by electromagnetic field in the system are examined. The effects of exciton-phonon and exciton-phonon-photon interactions on the band structure and formation of self-localized excitations are examined on various time scales. A new mechanism for controlling bandgap parameters in a bistable regime is described. Some effects of electromagnetic-field nonuniformity on generation of phonons in molecules and exciton self-localization are investigated

  18. Efficient singlet exciton fission in pentacene prepared from a soluble precursor

    Directory of Open Access Journals (Sweden)

    Maxim Tabachnyk

    2016-11-01

    Full Text Available Carrier multiplication using singlet exciton fission (SF to generate a pair of spin-triplet excitons from a single optical excitation has been highlighted as a promising approach to boost the photocurrent in photovoltaics (PVs thereby allowing PV operation beyond the Shockley-Queisser limit. The applicability of many efficient fission materials, however, is limited due to their poor solubility. For instance, while acene-based organics such as pentacene (Pc show high SF yields (up to200%, the plain acene backbone renders the organic molecule insoluble in common organic solvents. Previous approaches adding solubilizing side groups such as bis(tri-iso-propylsilylethynyl to the Pc core resulted in low vertical carrier mobilities due to reduction of the transfer integrals via steric hindrance, which prevented high efficiencies in PVs. Here we show how to achieve good solubility while retaining the advantages of molecular Pc by using a soluble precursor route. The precursor fully converts into molecular Pc through thermal removal of the solubilizing side groups upon annealing above 150 °C in the solid state. The annealed precursor shows small differences in the crystallinity compared to evaporated thin films of Pc, indicating that the Pc adopts the bulk rather than surface polytype. Furthermore, we identify identical SF properties such as sub-100 fs fission time and equally long triplet lifetimes in both samples.

  19. Nonlinear spectroscopy of the bound exciton states in CdSe single crystals

    International Nuclear Information System (INIS)

    Lisitsa, M.P.; Onishchenko, N.A.; Stolyarenko, A.V.; Ananchenko, V.V.; Polishchuk, S.V.

    1989-01-01

    The study is devoted to the pulsed laser radiation effect on the time-resolved variations of free and bound exciton bands region at the helium temperature. A gradual disappearance of the bound I 2 exciton state is observed with increase of the excitation intensity I in CdSe transmission spectra. This phenomenon is explained by the fact that despite of the shorter life of I 2 excitons as compared to the free ones, the concentration of the centres on which they localize is rather low (≤10 16 cm -3 ) while the evolution of the light-generated electron-hole pairs is such as the most probable recombination through the bound excitons. The transmission spectrum kinetics is studied. The intensity limitation of the laser pulse transmitted through the crystal in the region of the exciton ground state region is shown to be related with two-photon absorption (TPA) in which the exciton state is an intermediate level. The calculation results are in good agreement with the experiment. The estimations show the giant TPA coefficient of ∼10 3 cm/MW. The evolution of photoexcited nonequilibrium electron-hole pairs is studied. The possibility of using CdSe single crystals as spectrum-selective limiters of the laser pulses is shown. (author)

  20. Excitons in semiconducting quantum filaments of CdS and CdSe with dielectric barriers

    CERN Document Server

    Dneprovskij, V S; Shalygina, O A; Lyaskovskij, V L; Mulyarov, E A; Gavrilov, S A; Masumoto, I

    2002-01-01

    The peculiarities of the luminescence spectra obtained by different polarization and intensity of the pumping excitation and luminescence kinetics of the CdS and CdSe nanocrystals are explained by the exciton transitions in the semiconducting quantum threads with dielectric barriers. The exciton transition energies correspond to the calculated ones with an account of both their dimensional quantization and the effect of the excitons dielectric intensification. It is shown that the excitons transition energies do not change by the change in the quantum threads diameter within the wide range, while the increase in the one-dimensional forbidden zone width of quantum thread by the decrease in its diameter is compensated through the decrease in the excitons binding energy

  1. Influence of the core-hole effect on optical properties of magnesium oxide (MgO) near the Mg L-edge region.

    Science.gov (United States)

    Sinha, Mangalika; Modi, Mohammed H; Ghosh, Haranath; Yadav, P K; Gupta, R K

    2018-05-01

    The influence of the core-hole effect on optical properties of magnesium oxide (MgO) is established through experimental determination of optical constants and first-principles density functional theory studies. Optical constants (δ and β) of MgO thin film are measured in the spectral region 40-300 eV using reflectance spectroscopy techniques at the Indus-1 synchrotron radiation source. The obtained optical constants show strong core exciton features near the Mg L-edge region, causing significant mismatch with Henke's tabulated values. On comparing the experimentally obtained optical constants with Henke's tabulated values, an edge shift of ∼3.0 eV is also observed. Distinct evidence of effects of core exciton on optical constants (δ and β) in the near Mg L-edge absorption spectra are confirmed through first-principles simulations.

  2. Exceptionally slow rise in differential reflectivity spectra of excitons in GaN: effect of excitation-induced dephasing

    International Nuclear Information System (INIS)

    Stanton, C.J.; Kenrow, J.; El Sayed, K.; Jho, Y.D.; Kim, D.S.; Song, J.J.; Fischer, Arthur Joseph

    2004-01-01

    Femtosecond differential reflectivity spectroscopy (DRS) and four-wave mixing (FWM) experiments were performed simultaneously to study the initial temporal dynamics of the exciton line-shapes in GaN epilayers. Beats between the A-B excitons were found only for positive time delay in both DRS and FWM experiments. The rise time at negative time delay for the DRS was much slower than the FWM signal or differential transmission spectroscopy at the exciton resonance. A numerical solution of a six band semiconductor Bloch equation model including nonlinearities at the Hartree-Fock level shows that this slow rise in the DRS results from excitation induced dephasing, that is, the strong density dependence of the dephasing time which changes with the laser excitation energy.

  3. Dynamically controlling the emission of single excitons in photonic crystal cavities

    NARCIS (Netherlands)

    Pagliano, F.; Cho, Y.; Xia, T.; Otten, van F.W.M.; Johne, R.; Fiore, A.

    2014-01-01

    Single excitons in semiconductor microcavities represent a solid state and scalable platform for cavity quantum electrodynamics, potentially enabling an interface between flying (photon) and static (exciton) quantum bits in future quantum networks. While both singlephoton emission and the strong

  4. One dimensional models of excitons in carbon nanotubes

    DEFF Research Database (Denmark)

    Cornean, Horia Decebal; Duclos, P.; Pedersen, Thomas Garm

    Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable.......Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable....

  5. One-dimensional models of excitons in carbon nanotubes

    DEFF Research Database (Denmark)

    Cornean, Horia Decebal; Duclos, Pierre; Pedersen, Thomas Garm

    2004-01-01

    Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one-dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable.......Excitons in carbon nanotubes may be modeled by two oppositely charged particles living on the surface of a cylinder. We derive three one-dimensional effective Hamiltonians which become exact as the radius of the cylinder vanishes. Two of them are solvable....

  6. Signatures of exciton condensation in a transition metal dichalcogenide

    Science.gov (United States)

    Kogar, Anshul; Rak, Melinda S.; Vig, Sean; Husain, Ali A.; Flicker, Felix; Joe, Young Il; Venema, Luc; MacDougall, Greg J.; Chiang, Tai C.; Fradkin, Eduardo; van Wezel, Jasper; Abbamonte, Peter

    2017-12-01

    Bose condensation has shaped our understanding of macroscopic quantum phenomena, having been realized in superconductors, atomic gases, and liquid helium. Excitons are bosons that have been predicted to condense into either a superfluid or an insulating electronic crystal. Using the recently developed technique of momentum-resolved electron energy-loss spectroscopy (M-EELS), we studied electronic collective modes in the transition metal dichalcogenide semimetal 1T-TiSe2. Near the phase-transition temperature (190 kelvin), the energy of the electronic mode fell to zero at nonzero momentum, indicating dynamical slowing of plasma fluctuations and crystallization of the valence electrons into an exciton condensate. Our study provides compelling evidence for exciton condensation in a three-dimensional solid and establishes M-EELS as a versatile technique sensitive to valence band excitations in quantum materials.

  7. Disorder effects on free excitons in CdSsub(1-x)Sesub(x) mixed crystals

    International Nuclear Information System (INIS)

    Goede, O.; Hennig, D.; John, L.

    1979-01-01

    In CdSsub(1-x)Sesub(x) mixed crystals the energies and transition probability ratios for free A, B, and C excitons are obtained as a function of the composition x by reflection and emission measurements at 77 K. The observation of the disorder-allowed A(GAMMA 6 ) exciton transition, the bowing of the energy difference between A and C exciton, and the broadening of the exciton lines clearly demonstrate the importance of disorder effects in these mixed crystals. This conclusion is further supported by the stress-induced enhancement of the A(GAMMA 6 ) exciton transition probability by uniaxial stress parallel to the c-axis of the mixed crystals. The experimental results are discussed on the basis of an effective exciton Hamiltonian consisting of a quasi-cubic VCA-Hamiltonian for wurtzite-type mixed crystals and an additional lower-symmetric term which describes the disorder effects phenomenologically by two fluctuating crystal fields parallel and perpendicular to the c-axis, respectively. (author)

  8. Pure exciton- and magnon-assisted optical transitionsin the one-dimensional antiferromagnet CsMnCl3x2H2O (CMC)

    International Nuclear Information System (INIS)

    Jia, W.; Strauss, E.; Yen, W.M.

    1981-01-01

    We report the first observation of the pure electronic transitions in the 4 T 1 state of Mn 2+ ions in the one-dimensional antiferromagnet CsMnCl 3 x2H 2 O (CMC) in the absorption, excitation, and fluorescence spectra. Selection rules are analyzed: the exciton transition is electric dipole allowed, the magnon sideband in emission is a single-ion process, and is both electric and magnetic dipole allowed; however, the magnon sideband in absorption is an ion-pair process and is a weakened-electric-dipole and magnetic-dipole transition. The density of magnon states and the line profile of the magnon sideband have been calculated. The results explain the peculiar line shapes of the observed sideband emission. An exponential decay of the exciton is observed with a lifetime of 0.576 ms

  9. Importance of Electronic Correlations and Unusual Excitonic Effects in Formamidinium Lead Halide Perovskites

    Science.gov (United States)

    Whitcher, T. J.; Zhu, J.-X.; Chi, X.; Hu, H.; Zhao, Daming; Asmara, T. C.; Yu, X.; Breese, M. B. H.; Castro Neto, A. H.; Lam, Y. M.; Wee, A. T. S.; Chia, Elbert E. M.; Rusydi, A.

    2018-04-01

    Hybrid inorganic-organic perovskites have recently attracted much interest because of both rich fundamental sciences and potential applications such as the primary energy-harvesting material in solar cells. However, an understanding of electronic and optical properties, particularly the complex dielectric function, of these materials is still lacking. Here, we report on the electronic and optical properties of selective perovskites using temperature-dependent spectroscopic ellipsometry, x-ray absorption spectroscopy supported by first-principles calculations. Surprisingly, the perovskite FA0.85Cs0.15PbI2.9Br0.1 has a very high density of low-energy excitons that increases with increasing temperature even at room temperature, which is not seen in any other material. This is found to be due to the strong, unscreened electron-electron and partially screened electron-hole interactions, which then tightly connect low- and high-energy bands caused by doping.

  10. Importance of Electronic Correlations and Unusual Excitonic Effects in Formamidinium Lead Halide Perovskites

    Directory of Open Access Journals (Sweden)

    T. J. Whitcher

    2018-05-01

    Full Text Available Hybrid inorganic-organic perovskites have recently attracted much interest because of both rich fundamental sciences and potential applications such as the primary energy-harvesting material in solar cells. However, an understanding of electronic and optical properties, particularly the complex dielectric function, of these materials is still lacking. Here, we report on the electronic and optical properties of selective perovskites using temperature-dependent spectroscopic ellipsometry, x-ray absorption spectroscopy supported by first-principles calculations. Surprisingly, the perovskite FA_{0.85}Cs_{0.15}PbI_{2.9}Br_{0.1} has a very high density of low-energy excitons that increases with increasing temperature even at room temperature, which is not seen in any other material. This is found to be due to the strong, unscreened electron-electron and partially screened electron-hole interactions, which then tightly connect low- and high-energy bands caused by doping.

  11. Hydrostatic pressure and temperature effects of an exciton-donor complex in quantum dots

    International Nuclear Information System (INIS)

    Xie Wenfang

    2012-01-01

    Using the matrix diagonalization method and the compact density-matrix approach, we studied the combined effects of hydrostatic pressure and temperature on the electronic and optical properties of an exciton-donor complex in a disc-shaped quantum dot. We have calculated the binding energy and the oscillator strength of the intersubband transition from the ground state into the first excited state as a function of the dot radius. Based on the computed energies and wave functions, the linear, third-order nonlinear and total optical absorption coefficients as well as the refractive index have been examined. We find that the ground state binding energy and the oscillator strength are strongly affected by the quantum dot radius, hydrostatic pressure and temperature. The results also show that the linear, third-order nonlinear and total absorption coefficients and refractive index changes strongly depend on temperature and hydrostatic pressure.

  12. Programmed coherent coupling in a synthetic DNA-based excitonic circuit

    Science.gov (United States)

    Boulais, Étienne; Sawaya, Nicolas P. D.; Veneziano, Rémi; Andreoni, Alessio; Banal, James L.; Kondo, Toru; Mandal, Sarthak; Lin, Su; Schlau-Cohen, Gabriela S.; Woodbury, Neal W.; Yan, Hao; Aspuru-Guzik, Alán; Bathe, Mark

    2018-02-01

    Natural light-harvesting systems spatially organize densely packed chromophore aggregates using rigid protein scaffolds to achieve highly efficient, directed energy transfer. Here, we report a synthetic strategy using rigid DNA scaffolds to similarly program the spatial organization of densely packed, discrete clusters of cyanine dye aggregates with tunable absorption spectra and strongly coupled exciton dynamics present in natural light-harvesting systems. We first characterize the range of dye-aggregate sizes that can be templated spatially by A-tracts of B-form DNA while retaining coherent energy transfer. We then use structure-based modelling and quantum dynamics to guide the rational design of higher-order synthetic circuits consisting of multiple discrete dye aggregates within a DX-tile. These programmed circuits exhibit excitonic transport properties with prominent circular dichroism, superradiance, and fast delocalized exciton transfer, consistent with our quantum dynamics predictions. This bottom-up strategy offers a versatile approach to the rational design of strongly coupled excitonic circuits using spatially organized dye aggregates for use in coherent nanoscale energy transport, artificial light-harvesting, and nanophotonics.

  13. Strong excitonic interactions in the oxygen K-edge of perovskite oxides.

    Science.gov (United States)

    Tomita, Kota; Miyata, Tomohiro; Olovsson, Weine; Mizoguchi, Teruyasu

    2017-07-01

    Excitonic interactions of the oxygen K-edge electron energy-loss near-edge structure (ELNES) of perovskite oxides, CaTiO 3 , SrTiO 3 , and BaTiO 3 , together with reference oxides, MgO, CaO, SrO, BaO, and TiO 2 , were investigated using a first-principles Bethe-Salpeter equation calculation. Although the transition energy of oxygen K-edge is high, strong excitonic interactions were present in the oxygen K-edge ELNES of the perovskite oxides, whereas the excitonic interactions were negligible in the oxygen K-edge ELNES of the reference compounds. Detailed investigation of the electronic structure suggests that the strong excitonic interaction in the oxygen K-edge ELNES of the perovskite oxides is caused by the directionally confined, low-dimensional electronic structure at the Ti-O-Ti bonds. Copyright © 2016 Elsevier B.V. All rights reserved.

  14. Exciton delocalization incorporated drift-diffusion model for bulk-heterojunction organic solar cells

    Science.gov (United States)

    Wang, Zi Shuai; Sha, Wei E. I.; Choy, Wallace C. H.

    2016-12-01

    Modeling the charge-generation process is highly important to understand device physics and optimize power conversion efficiency of bulk-heterojunction organic solar cells (OSCs). Free carriers are generated by both ultrafast exciton delocalization and slow exciton diffusion and dissociation at the heterojunction interface. In this work, we developed a systematic numerical simulation to describe the charge-generation process by a modified drift-diffusion model. The transport, recombination, and collection of free carriers are incorporated to fully capture the device response. The theoretical results match well with the state-of-the-art high-performance organic solar cells. It is demonstrated that the increase of exciton delocalization ratio reduces the energy loss in the exciton diffusion-dissociation process, and thus, significantly improves the device efficiency, especially for the short-circuit current. By changing the exciton delocalization ratio, OSC performances are comprehensively investigated under the conditions of short-circuit and open-circuit. Particularly, bulk recombination dependent fill factor saturation is unveiled and understood. As a fundamental electrical analysis of the delocalization mechanism, our work is important to understand and optimize the high-performance OSCs.

  15. The confinement effect in spherical inhomogeneous quantum dots and stability of excitons

    Directory of Open Access Journals (Sweden)

    F. Benhaddou

    2017-06-01

    Full Text Available We investigate in this work the quantum confinement effect of exciton in spherical inhomogeneous quantum dots IQDs. The spherical core is enveloped by two shells. The inner shell is a semiconductor characterized by a small band-gap. The core and the outer shell are the same semiconductor characterized by a large band-gap. So there is a significant gap-offset creating a deep potential well where the excitons are localized and strongly confined. We have adopted the Ritz variational method to calculate numerically the excitonic ground state energy and its binding energy in the strong, moderate and low confinement regimes. The results show that the Ritz variational method is in good agreement with the perturbation method in strong confinement. There is a double confinement effect and dual control. The calculation checks the effective Rydberg R* at the asymptotic limit of bulk semiconductor when the thickness takes very large values. The excitonic binding energy increases, Thus giving the excitons a high stability even at ambient temperature. These nanosystems are promising in several applications: lighting, detection, biological labeling and quantum computing.

  16. The Dual Role of Disorder on the Dissociation of Interfacial Charge Transfer Excitons

    Science.gov (United States)

    Shi, Liang; Lee, Chee-Kong; Willard, Adam

    In organic-based photovoltaics (OPV), dissociation of neutral photo-excitations (i.e., Frenkel excitons) into free charge carriers requires the excitons to overcome binding energy that can significantly exceed thermal energies. The inability of bound charges to overcome this large binding energy has been implicated as a primary source of efficiency loss in OPVs. Despite the potential impact on the performance of organic solar cells much remains to be understood about the microscopic mechanism of exciton dissociation in OPV materials. Here we explore the role of static molecular disorder in mediating this charge dissociation process. Using a simple lattice model of exciton dynamics we demonstrate that random spatial variations in the energetic landscape can mitigate the effects of the exciton binding energy by lowering the free energy barrier. By considering the competition between this thermodynamic effect and the disorder-induced slowing of dissociation kinetics we demonstrate that exciton dissociation yields are expected to depend non-monotonically on the degree of static disorder. We conclude that a certain amount of molecular-scale disorder is desirable in order to optimize the performance of organic photovoltaic materials.

  17. Triplet energy transfer and triplet exciton recycling in singlet fission sensitized organic heterojunctions

    Science.gov (United States)

    Hamid, Tasnuva; Yambem, Soniya D.; Crawford, Ross; Roberts, Jonathan; Pandey, Ajay K.

    2017-08-01

    Singlet exciton fission is a process where an excited singlet state splits into two triplets, thus leading to generation of multiple excitons per absorbed photon in organic semiconductors. Herein, we report a detailed exciton management approach for multiexciton harvesting over a broadband region of the solar spectrum in singlet fission sensitized organic photodiodes. Through systematic studies on the model cascade of pentacene/rubrene/C60, we found that efficient photocurrent generation from pentacene can still occur despite the presence of a >10nm thick interlayer of rubrene in between the pentacene/C60 heterojunction. Our results show that thin rubrene interlayers of thickness pentacene despite having a reasonably thick rubrene interlayer, that too with higher triplet energy (T1=1.12 eV) than pentacene (T1= 0.86 eV), makes its operation a rather interesting result. We discuss the role of rubrene interlayer film discontinuity, triplet exciton reflection from rubrene interlayer and triplet energy transfer from rubrene to pentacene layer followed by diffusion of triplet excitons through rubrene as plausible mechanisms that would enable triplet excitons from pentacene to generate significant photocurrent in a multilayer organic heterojunction.

  18. Efficient Exciton Diffusion and Resonance-Energy Transfer in Multi-Layered Organic Epitaxial Nanofibers

    DEFF Research Database (Denmark)

    Tavares, Luciana; Cadelano, Michele; Quochi, Francesco

    2015-01-01

    Multi-layered epitaxial nanofibers are exemplary model systems for the study of exciton dynamics and lasing in organic materials due to their well-defined morphology, high luminescence efficiencies, and color tunability. We resort to temperature-dependent cw and picosecond photoluminescence (PL......) spectroscopy to quantify exciton diffusion and resonance-energy transfer (RET) processes in multi-layered nanofibers consisting of alternating layers of para-hexaphenyl (p6P) and α-sexithiophene (6T), serving as exciton donor and acceptor material, respectively. The high probability for RET processes...... is confirmed by Quantum Chemical calculations. The activation energy for exciton diffusion in p6P is determined to be as low as 19 meV, proving p6P epitaxial layers also as a very suitable donor material system. The small activation energy for exciton diffusion of the p6P donor material, the inferred high p6P...

  19. Excitons in intact cells of photosynthetic bacteria.

    Science.gov (United States)

    Freiberg, Arvi; Pajusalu, Mihkel; Rätsep, Margus

    2013-09-26

    Live cells and regular crystals seem fundamentally incompatible. Still, effects characteristic to ideal crystals, such as coherent sharing of excitation, have been recently used in many studies to explain the behavior of several photosynthetic complexes, especially the inner workings of the light-harvesting apparatus of the oldest known photosynthetic organisms, the purple bacteria. To this date, there has been no concrete evidence that the same effects are instrumental in real living cells, leaving a possibility that this is an artifact of unnatural study conditions, not a real effect relevant to the biological operation of bacteria. Hereby, we demonstrate survival of collective coherent excitations (excitons) in intact cells of photosynthetic purple bacteria. This is done by using excitation anisotropy spectroscopy for tracking the temperature-dependent evolution of exciton bands in light-harvesting systems of increasing structural complexity. The temperature was gradually raised from 4.5 K to ambient temperature, and the complexity of the systems ranged from detergent-isolated complexes to complete bacterial cells. The results provide conclusive evidence that excitons are indeed one of the key elements contributing to the energetic and dynamic properties of photosynthetic organisms.

  20. Effect of localized surface-plasmon mode on exciton transport and radiation emission in carbon nanotubes.

    Science.gov (United States)

    Roslyak, Oleksiy; Cherqui, Charles; Dunlap, David H; Piryatinski, Andrei

    2014-07-17

    We report on a general theoretical approach to study exciton transport and emission in a single-walled carbon nanotube (SWNT) in the presence of a localized surface-plasmon (SP) mode within a metal nanoparticle interacting via near-field coupling. We derive a set of quantum mechanical equations of motion and approximate rate equations that account for the exciton, SP, and the environmental degrees of freedom. The material equations are complemented by an expression for the radiated power that depends on the exciton and SP populations and coherences, allowing for an examination of the angular distribution of the emitted radiation that would be measured in experiment. Numerical simulations for a (6,5) SWNT and cone-shaped Ag metal tip (MT) have been performed using this methodology. Comparison with physical parameters shows that the near-field interaction between the exciton-SP occurs in a weak coupling regime, with the diffusion processes being much faster than the exciton-SP population exchange. In such a case, the effect of the exciton population transfer to the MT with its subsequent dissipation (i.e., the Förster energy transfer) is to modify the exciton steady state distribution while reducing the equilibration time for excitons to reach a steady sate distribution. We find that the radiation distribution is dominated by SP emission for a SWNT-MT separation of a few tens of nanometers due to the fast SP emission rate, whereas the exciton-SP coherences can cause its rotation.

  1. Surface strain engineering through Tb doping to study the pressure dependence of exciton-phonon coupling in ZnO nanoparticles

    International Nuclear Information System (INIS)

    Sharma, A.; Dhar, S.; Singh, B. P.; Nayak, C.; Bhattacharyya, D.; Jha, S. N.

    2013-01-01

    A compressive hydrostatic strain has been found to develop in the ZnO lattice as a result of accumulation of Tb ions on the surface of the nanoparticles for Tb mole-fraction less than 0.04. This hydrostatic strain can be controlled up to ≈14 GPa by varying the Tb mole-fraction. Here, we have utilized this novel technique of surface strain engineering through Tb doping for introducing hydrostatic compressive strain in the lattice to study the pressure dependent electronic and vibrational properties of ZnO nanoparticles. Our study reveals that when subjected to pressure, nanoparticles of ZnO behave quite differently than bulk in many aspects. Unlike bulk ZnO, which is reported to go through a wurtzite to rock-salt structural phase transition at ≈8 GPa, ZnO nanoparticles do not show such transition and remain in wurtzite phase even at 14 GPa of pressure. Furthermore, the Grüneisen parameters for the optical phonon modes are found to be order of magnitude smaller in ZnO nanoparticles as compared to bulk. Our study also suggests an increase of the dielectric constant with pressure, which is opposite to what has been reported for bulk ZnO. Interestingly, it has also been found that the exciton-phonon interaction depends strongly upon pressure in this system. The exciton-phonon coupling has been found to decrease as pressure increases. A variational technique has been adopted to theoretically calculate the exciton-LO phonon coupling coefficient in ZnO nanoparticles as a function of pressure, which shows a good agreement with the experimental results. These findings imply that surface engineering of ZnO nanoparticles with Tb could indeed be an efficient tool to enhance and control the optical performance of this material

  2. Surface strain engineering through Tb doping to study the pressure dependence of exciton-phonon coupling in ZnO nanoparticles

    Energy Technology Data Exchange (ETDEWEB)

    Sharma, A.; Dhar, S., E-mail: dhar@phy.iitb.ac.in; Singh, B. P. [Physics Department, Indian Institute of Technology Bombay, Powai, Mumbai 400076 (India); Nayak, C.; Bhattacharyya, D. [Applied Spectroscopy Division, Bhabha Atomic Research Centre, Mumbai-400085 (India); Jha, S. N. [Raja Ramanna Centre for Advanced Technology (RRCAT), Indore (India)

    2013-12-07

    A compressive hydrostatic strain has been found to develop in the ZnO lattice as a result of accumulation of Tb ions on the surface of the nanoparticles for Tb mole-fraction less than 0.04. This hydrostatic strain can be controlled up to ≈14 GPa by varying the Tb mole-fraction. Here, we have utilized this novel technique of surface strain engineering through Tb doping for introducing hydrostatic compressive strain in the lattice to study the pressure dependent electronic and vibrational properties of ZnO nanoparticles. Our study reveals that when subjected to pressure, nanoparticles of ZnO behave quite differently than bulk in many aspects. Unlike bulk ZnO, which is reported to go through a wurtzite to rock-salt structural phase transition at ≈8 GPa, ZnO nanoparticles do not show such transition and remain in wurtzite phase even at 14 GPa of pressure. Furthermore, the Grüneisen parameters for the optical phonon modes are found to be order of magnitude smaller in ZnO nanoparticles as compared to bulk. Our study also suggests an increase of the dielectric constant with pressure, which is opposite to what has been reported for bulk ZnO. Interestingly, it has also been found that the exciton-phonon interaction depends strongly upon pressure in this system. The exciton-phonon coupling has been found to decrease as pressure increases. A variational technique has been adopted to theoretically calculate the exciton-LO phonon coupling coefficient in ZnO nanoparticles as a function of pressure, which shows a good agreement with the experimental results. These findings imply that surface engineering of ZnO nanoparticles with Tb could indeed be an efficient tool to enhance and control the optical performance of this material.

  3. Theoretical study of excitonic complexes in semiconductors quantum wells

    International Nuclear Information System (INIS)

    Dacal, Luis Carlos Ogando

    2001-08-01

    A physical system where indistinguishable particles interact with each other creates the possibility of studying correlation and exchange effect. The simplest system is that one with only two indistinguishable particles. In condensed matter physics, these complexes are represented by charged excitons, donors and acceptors. In quantum wells, the valence band is not parabolic, therefore, the negatively charged excitons and donors are theoretically described in a simpler way. Despite the fact that the stability of charged excitons (trions) is known since the late 50s, the first experimental observation occurred only at the early 90s in quantum well samples, where their binding energies are one order of magnitude larger due to the one dimensional carriers confinement. After this, these complexes became the subject of an intense research because the intrinsic screening of electrical interactions in semiconductor materials allows that magnetic fields that are usual in laboratories have strong effects on the trion binding energy. Another rich possibility is the study of trions as an intermediate state between the neutral exciton and the Fermi edge singularity when the excess of doping carriers is increased. In this thesis, we present a theoretical study of charged excitons and negatively charged donors in GaAs/Al 0.3 Ga 0.7 As quantum wells considering the effects of external electric and magnetic fields. We use a simple, accurate and physically clear method to describe these systems in contrast with the few and complex treatments s available in the literature. Our results show that the QW interface defects have an important role in the trion dynamics. This is in agreement with some experimental works, but it disagrees with other ones. (author)

  4. Multicomponent exciton gas in cuprous oxide: cooling behaviour and the role of Auger decay

    Science.gov (United States)

    Semkat, D.; Sobkowiak, S.; Schöne, F.; Stolz, H.; Koch, Th; Fehske, H.

    2017-10-01

    In this paper we present a hydrodynamic model to describe the dynamics of para- and orthoexcitons in cuprous oxide at ultralow temperatures inside a stress induced potential trap. We take into account the finite lifetime of the excitons, the excitation process and exciton-phonon as well as exciton-exciton interaction. Furthermore, we model the two-body loss mechanism assuming an Auger-like effect and compare it to an alternative explanation which relies on the formation of biexcitons. We discuss in detail the influence on the numerical results and compare the predictions to experimental data.

  5. Synthesis, structural, thermal and optical studies of inorganic-organic hybrid semiconductors, R-PbI4

    Science.gov (United States)

    Pradeesh, K.; Nageswara Rao, K.; Vijaya Prakash, G.

    2013-02-01

    Wide varieties of naturally self-assembled two-dimensional inorganic-organic (IO) hybrid semiconductors, (4-ClC6H4NH3)2PbI4, (C6H9C2H4NH3)2PbI4, (CnH2n+1NH3)2PbI4 (where n = 12, 16, 18), (CnH2n-1NH3)2PbI4 (where n = 3, 4, 5), (C6H5C2H4NH3)2PbI4, NH3(CH2)12NH3PbI4, and (C4H3SC2H4NH3)2PbI4, were fabricated by intercalating structurally diverse organic guest moieties into lead iodide perovskite structure. The crystal packing of all these fabricated IO-hybrids comprises of well-ordered organic and inorganic layers, stacked-up alternately along c-axis. Almost all these hybrids are thermally stable upto 200 °C and show strong room-temperature exciton absorption and photoluminescence features. These strongly confined optical excitons are highly influenced by structural deformation of PbI matrix due to the conformation of organic moiety. A systematic correlation of optical exciton behavior of IO-hybrids with the organic/inorganic layer thicknesses, intercalating organic moieties, and various structural disorders were discussed. This systematic study clearly suggests that the PbI layer crumpling is directly responsible for the tunability of optical exciton energy.

  6. Observation of the exciton and Urbach band tail in low-temperature-grown GaAs using four-wave mixing spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Webber, D.; Yildirim, M.; Hacquebard, L.; March, S.; Mathew, R.; Gamouras, A.; Hall, K. C. [Department of Physics and Atmospheric Science, Dalhousie University, Halifax, Nova Scotia B3H 4R2 (Canada); Liu, X.; Dobrowolska, M.; Furdyna, J. K. [Department of Physics, University of Notre Dame, Notre Dame, Indiana 46556 (United States)

    2014-11-03

    Four-wave mixing (FWM) spectroscopy reveals clear signatures associated with the exciton, free carrier inter-band transitions, and the Urbach band tail in low-temperature-grown GaAs, providing a direct measure of the effective band gap as well as insight into the influence of disorder on the electronic structure. The ability to detect (and resolve) these contributions, in contrast to linear spectroscopy, is due to an enhanced sensitivity of FWM to the optical joint density of states and to many-body effects. Our experiments demonstrate the power of FWM for studying the near-band-edge optical properties and coherent carrier dynamics in low-temperature-grown semiconductors.

  7. Singlet exciton fission in polycrystalline pentacene: from photophysics toward devices.

    Science.gov (United States)

    Wilson, Mark W B; Rao, Akshay; Ehrler, Bruno; Friend, Richard H

    2013-06-18

    Singlet exciton fission is the process in conjugated organic molecules bywhich a photogenerated singlet exciton couples to a nearby chromophore in the ground state, creating a pair of triplet excitons. Researchers first reported this phenomenon in the 1960s, an event that sparked further studies in the following decade. These investigations used fluorescence spectroscopy to establish that exciton fission occurred in single crystals of several acenes. However, research interest has been recently rekindled by the possibility that singlet fission could be used as a carrier multiplication technique to enhance the efficiency of photovoltaic cells. The most successful architecture to-date involves sensitizing a red-absorbing photoactive layer with a blue-absorbing material that undergoes fission, thereby generating additional photocurrent from higher-energy photons. The quest for improved solar cells has spurred a drive to better understand the fission process, which has received timely aid from modern techniques for time-resolved spectroscopy, quantum chemistry, and small-molecule device fabrication. However, the consensus interpretation of the initial studies using ultrafast transient absorption spectroscopy was that exciton fission was suppressed in polycrystalline thin films of pentacene, a material that would be otherwise expected to be an ideal model system, as well as a viable candidate for fission-sensitized photovoltaic devices. In this Account, we review the results of our recent transient absorption and device-based studies of polycrystalline pentacene. We address the controversy surrounding the assignment of spectroscopic features in transient absorption data, and illustrate how a consistent interpretation is possible. This work underpins our conclusion that singlet fission in pentacene is extraordinarily rapid (∼80 fs) and is thus the dominant decay channel for the photoexcited singlet exciton. Further, we discuss our demonstration that triplet excitons

  8. Tuning crystalline ordering by annealing and additives to study its effect on exciton diffusion in a polyalkylthiophene copolymer.

    Science.gov (United States)

    Chowdhury, Mithun; Sajjad, Muhammad T; Savikhin, Victoria; Hergué, Noémie; Sutija, Karina B; Oosterhout, Stefan D; Toney, Michael F; Dubois, Philippe; Ruseckas, Arvydas; Samuel, Ifor D W

    2017-05-17

    The influence of various processing conditions on the singlet exciton diffusion is explored in films of a conjugated random copolymer poly-(3-hexylthiophene-co-3-dodecylthiophene) (P3HT-co-P3DDT) and correlated with the degree of crystallinity probed by grazing incidence X-ray scattering and with exciton bandwidth determined from absorption spectra. The exciton diffusion coefficient is deduced from exciton-exciton annihilation measurements and is found to increase by more than a factor of three when thin films are annealed using CS 2 solvent vapour. A doubling of exciton diffusion coefficient is observed upon melt annealing at 200 °C and the corresponding films show about 50% enhancement in the degree of crystallinity. In contrast, films fabricated from polymer solutions containing a small amount of either solvent additive or nucleating agent show a decrease in exciton diffusion coefficient possibly due to formation of traps for excitons. Our results suggest that the enhancement of exciton diffusivity occurs because of increased crystallinity of alkyl-stacking and longer conjugation of aggregated chains which reduces the exciton bandwidth.

  9. Multi-Excitonic Quantum Dot Molecules

    Science.gov (United States)

    Scheibner, M.; Stinaff, E. A.; Doty, M. F.; Ware, M. E.; Bracker, A. S.; Gammon, D.; Ponomarev, I. V.; Reinecke, T. L.; Korenev, V. L.

    2006-03-01

    With the ability to create coupled pairs of quantum dots, the next step towards the realization of semiconductor based quantum information processing devices can be taken. However, so far little knowledge has been gained on these artificial molecules. Our photoluminescence experiments on single InAs/GaAs quantum dot molecules provide the systematics of coupled quantum dots by delineating the spectroscopic features of several key charge configurations in such quantum systems, including X, X^+,X^2+, XX, XX^+ (with X being the neutral exciton). We extract general rules which determine the formation of molecular states of coupled quantum dots. These include the fact that quantum dot molecules provide the possibility to realize various spin configurations and to switch the electron hole exchange interaction on and off by shifting charges inside the molecule. This knowledge will be valuable in developing implementations for quantum information processing.

  10. Thermalization of Hot Free Excitons in ZnSe-Based Quantum Wells

    DEFF Research Database (Denmark)

    Hoffmann, J.; Umlauff, M.; Kalt, H.

    1997-01-01

    Thermalization of hot-exciton populations in ZnSe quantum wells occurs on a time scale of 100 ps. Strong exciton-phonon coupling in II-VI semiconductors leads to a direct access to the thermalization dynamics via time-resolved spectroscopy of phonon-assisted luminescence. The experimental spectra...

  11. Magnetic exciton dispersion in praseodymium

    DEFF Research Database (Denmark)

    Rainford, B. D.; Houmann, Jens Christian Gylden

    1971-01-01

    Measurements of the dispersion of magnetic excitons have been made in a single crystal of praseodymium metal using inelastic neutron scattering. A preliminary analysis of the data yields the first detailed information about the exchange interactions and the crystal field splittings in the light...... rare-earth metals....

  12. How exciton-vibrational coherences control charge separation in the photosystem II reaction center.

    Science.gov (United States)

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

    2015-12-14

    In photosynthesis absorbed sun light produces collective excitations (excitons) that form a coherent superposition of electronic and vibrational states of the individual pigments. Two-dimensional (2D) electronic spectroscopy allows a visualization of how these coherences are involved in the primary processes of energy and charge transfer. Based on quantitative modeling we identify the exciton-vibrational coherences observed in 2D photon echo of the photosystem II reaction center (PSII-RC). We find that the vibrations resonant with the exciton splittings can modify the delocalization of the exciton states and produce additional states, thus promoting directed energy transfer and allowing a switch between the two charge separation pathways. We conclude that the coincidence of the frequencies of the most intense vibrations with the splittings within the manifold of exciton and charge-transfer states in the PSII-RC is not occurring by chance, but reflects a fundamental principle of how energy conversion in photosynthesis was optimized.

  13. Generation and decay dynamics of triplet excitons in Alq3 thin films under high-density excitation conditions.

    Science.gov (United States)

    Watanabe, Sadayuki; Furube, Akihiro; Katoh, Ryuzi

    2006-08-31

    We studied the generation and decay dynamics of triplet excitons in tris-(8-hydroxyquinoline) aluminum (Alq3) thin films by using transient absorption spectroscopy. Absorption spectra of both singlet and triplet excitons in the film were identified by comparison with transient absorption spectra of the ligand molecule (8-hydroxyquinoline) itself and the excited triplet state in solution previously reported. By measuring the excitation light intensity dependence of the absorption, we found that exciton annihilation dominated under high-density excitation conditions. Annihilation rate constants were estimated to be gammaSS = (6 +/- 3) x 10(-11) cm3 s(-1) for single excitons and gammaTT = (4 +/- 2) x 10(-13) cm3 s(-1) for triplet excitons. From detailed analysis of the light intensity dependence of the quantum yield of triplet excitons under high-density conditions, triplet excitons were mainly generated through fission from highly excited singlet states populated by singlet-singlet exciton annihilation. We estimated that 30% of the highly excited states underwent fission.

  14. Correlation effect of Rabi oscillations of excitons in quantum dots

    International Nuclear Information System (INIS)

    Ishi-Hayase, J.; Akahane, K.; Yamamoto, Y.; Kujiraoka, M.; Ema, K.; Sasaki, M.

    2008-01-01

    We performed a transient four-wave mixing experiment on a strain-compensated InAs quantum dot (QD) ensemble over a wide range of excitation intensities. Under the resonant excitation of an exciton ground state, an extremely long dephasing time of 1 ns was found. By increasing the areas of the excitation pulses, Rabi oscillations of excitonic polarizations were clearly observed. The corresponding Rabi frequency is three orders of magnitude higher than the measured dephasing rate. For larger pulse areas, we found that the deviation of experimental data from two-level predictions became significant. The deviations cannot be explained by taking into account, as has been suggested in other research, excitation density-dependent dephasing or Hartree-Fock-type Coulomb interactions between excitons

  15. Stark effect of excitons in corrugated lateral surface superlattices: effect of centre-of-mass quantization

    International Nuclear Information System (INIS)

    Hong Sun

    1998-11-01

    The quantum confined Stark effect (QCSE) of excitons in GaAs/AlAs corrugated lateral surface superlattices (CLSSLs) is calculated. Blue and red shifts in the exciton energies are predicted for the heavy- and light-excitons in the CLSSLs, respectively, comparing with those in the unmodulated quantum well due to the different effective hole masses in the parallel direction. Sensitive dependence of the QCSE on the hole effective mass in the parallel direction is expected because of the ''centre-of-mass'' quantization (CMQ) induced by the periodic corrugated interfaces of the CLSSLs. The effect of the CMQ on the exciton mini-bands and the localization of the excitons in the CLSSLs is discussed. (author)

  16. Quantum Logic Using Excitonic Quantum Dots in External Optical Microcavities

    National Research Council Canada - National Science Library

    Raymer, Michael

    2003-01-01

    An experimental project was undertaken to develop means to achieve quantum optical strong coupling between a single GaAs quantum dot and the optical mode of a microcavity for the purpose of quantum...

  17. Optical Signatures of Coupled Quantum Dots

    Science.gov (United States)

    Stinaff, E. A.; Scheibner, M.; Bracker, A. S.; Ponomarev, I. V.; Korenev, V. L.; Ware, M. E.; Doty, M. F.; Reinecke, T. L.; Gammon, D.

    2006-02-01

    An asymmetric pair of coupled InAs quantum dots is tuned into resonance by applying an electric field so that a single hole forms a coherent molecular wave function. The optical spectrum shows a rich pattern of level anticrossings and crossings that can be understood as a superposition of charge and spin configurations of the two dots. Coulomb interactions shift the molecular resonance of the optically excited state (charged exciton) with respect to the ground state (single charge), enabling light-induced coupling of the quantum dots. This result demonstrates the possibility of optically coupling quantum dots for application in quantum information processing.

  18. Probing Exciton Diffusion and Dissociation in Single-Walled Carbon Nanotube-C60 Heterojunctions

    Energy Technology Data Exchange (ETDEWEB)

    Dowgiallo, Anne-Marie; Mistry, Kevin S.; Johnson, Justin C.; Reid, Obadiah G.; Blackburn, Jeffrey L.

    2016-05-19

    The efficiency of thin-film organic photovoltaic (OPV) devices relies heavily upon the transport of excitons to type-II heterojunction interfaces, where there is sufficient driving force for exciton dissociation and ultimately the formation of charge carriers. Semiconducting single-walled carbon nanotubes (SWCNTs) are strong near-infrared absorbers that form type-II heterojunctions with fullerenes such as C60. Although the efficiencies of SWCNT-fullerene OPV devices have climbed over the past few years, questions remain regarding the fundamental factors that currently limit their performance. In this study, we determine the exciton diffusion length in the C60 layer of SWCNT-C60 bilayer active layers using femtosecond transient absorption measurements. We demonstrate that hole transfer from photoexcited C60 molecules to SWCNTs can be tracked by the growth of narrow spectroscopic signatures of holes in the SWCNT 'reporter layer'. In bilayers with thick C60 layers, the SWCNT charge-related signatures display a slow rise over hundreds of picoseconds, reflecting exciton diffusion through the C60 layer to the interface. A model based on exciton diffusion with a Beer-Lambert excitation profile, as well as Monte Carlo simulations, gives the best fit to the data as a function of C60 layer thickness using an exciton diffusion length of approximately 5 nm.

  19. Optically detected cyclotron resonance in a single GaAs/AlGaAs heterojunction

    Energy Technology Data Exchange (ETDEWEB)

    Bartsch, Gregor

    2011-09-23

    Optically detected far-infrared cyclotron resonance (FIR-ODCR) in GaAs/AlGaAs HJs is interpreted in the frame of an exciton-dissociation mechanism. It is possible to explain the ODR mechanism by an exciton drag, mediated by ballistically propagating phonons. Furthermore, very narrow resonances are presented and realistic electron mobility values can be calculated. The exceptionally narrow ODCRs allow to measure conduction-band nonparabolicity effects and resolve satellite resonances, close to the main cyclotron resonance line.

  20. Exciton binding energy in wurtzite InGaN/GaN quantum wells

    International Nuclear Information System (INIS)

    Park, Seoung-Hwan; Kim, Jong-Jae; Kim, Hwa-Min

    2004-01-01

    The internal field and carrier density effects on the exciton binding energies in wurtzite (WZ) InGaN/GaN quantum-well (QW) structures are investigated using the multiband effective-mass theory, and are compared with those obtained from the at-band model and with those of GaN/AlGaN QW structures. The exciton binding energy is significantly reduced with increasing sheet carrier density, suggesting that excitons are nearly bleached at densities around 10 12 cm -2 for both InGaN/GaN and GaN/AlGaN QW structures. With the inclusion of the internal field, the exciton binding energy is substantialy reduced compared to that of the at-band model in the investigated region of the wells. This can be explained by a decrease in the momentum matrix element and an increase in the inverse screening length due to the internal field. The exciton binding energy of the InGaN/GaN structure is smaller than that of the GaN/AlGaN structure because InGaN/GaN structures have a smaller momentum matrix element and a larger inverse screening length than GaN/AlGaN structures.

  1. Correlated lifetimes of free paraexcitons and excitons trapped at oxygen vacancies in cuprous oxide

    International Nuclear Information System (INIS)

    Koirala, Sandhaya; Naka, Nobuko; Tanaka, Koichiro

    2013-01-01

    We have studied transients of luminescence due to free excitons and excitons trapped at oxygen vacancies in cuprous oxide. We find that both trapped and free paraexcitons have lifetime dependent on temperature and on the oxygen concentration. By using samples containing much less copper vacancies relative to oxygen vacancies, we find out the direct correlation between the free paraexciton lifetime and trapped exciton lifetime. - Highlights: ► We have investigated trapping of free excitons at oxygen vacancies in cuprous oxide. ► Lifetimes of free and trapped excitons exhibit correlative temperature dependence. ► Four-level model with the activation energy of 33 meV well explains the observation. ► Comparison is made using the four samples with different vacancy concentrations. ► We clarified the crucial role of the oxygen vacancy in shortening the lifetimes.

  2. Exciton absorption of entangled photons in semiconductor quantum wells

    Science.gov (United States)

    Rodriguez, Ferney; Guzman, David; Salazar, Luis; Quiroga, Luis; Condensed Matter Physics Group Team

    2013-03-01

    The dependence of the excitonic two-photon absorption on the quantum correlations (entanglement) of exciting biphotons by a semiconductor quantum well is studied. We show that entangled photon absorption can display very unusual features depending on space-time-polarization biphoton parameters and absorber density of states for both bound exciton states as well as for unbound electron-hole pairs. We report on the connection between biphoton entanglement, as quantified by the Schmidt number, and absorption by a semiconductor quantum well. Comparison between frequency-anti-correlated, unentangled and frequency-correlated biphoton absorption is addressed. We found that exciton oscillator strengths are highly increased when photons arrive almost simultaneously in an entangled state. Two-photon-absorption becomes a highly sensitive probe of photon quantum correlations when narrow semiconductor quantum wells are used as two-photon absorbers. Research funds from Facultad de Ciencias, Universidad de los Andes

  3. H-point exciton transitions in bulk MoS2

    International Nuclear Information System (INIS)

    Saigal, Nihit; Ghosh, Sandip

    2015-01-01

    Reflectance and photoreflectance spectrum of bulk MoS 2 around its direct bandgap energy have been measured at 12 K. Apart from spectral features due to the A and B ground state exciton transitions at the K-point of the Brillouin zone, one observes additional features at nearby energies. Through lineshape analysis the character of two prominent additional features are shown to be quite different from that of A and B. By comparing with reported electronic band structure calculations, these two additional features are identified as ground state exciton transitions at the H-point of the Brillouin zone involving two spin-orbit split valance bands. The excitonic energy gap at the H-point is 1.965 eV with a valance bands splitting of 185 meV. While at the K-point, the corresponding values are 1.920 eV and 205 meV, respectively

  4. 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.

  5. Frequency dependence of the radiative decay rate of excitons in self-assembled quantum dots: Experiment and theory

    DEFF Research Database (Denmark)

    Stobbe, Søren; Johansen, Jeppe; Kristensen, Philip Trøst

    2009-01-01

    We analyze time-resolved spontaneous emission from excitons confined in self-assembled InAs quantum dots placed at various distances to a semiconductor-air interface. The modification of the local density of optical states due to the proximity of the interface enables unambiguous determination...... furthermore discuss three models of quantum dot strain and compare the measured wave-function overlap to these models. The observed frequency dependence of the wave-function overlap can be understood qualitatively in terms of the different compressibility of electrons and holes originating from...

  6. PbSe Nanocrystal Excitonic Solar Cells

    KAUST Repository

    Choi, Joshua J.; Lim, Yee-Fun; Santiago-Berrios, Mitk’ El B.; Oh, Matthew; Hyun, Byung-Ryool; Sun, Liangfeng; Bartnik, Adam C.; Goedhart, Augusta; Malliaras, George G.; Abruña, Héctor D.; Wise, Frank W.; Hanrath, Tobias

    2009-01-01

    that Is distinct from previously reported Schottky devices and consistent with signatures of excitonic solar cells. Remarkably, despite the limitation of planar junction structure, and without film thickness optimization, the best performing device shows a 1-sun

  7. Exciton behavior in GaAs/AlGaAs coupled double quantum wells with interface disorder

    Energy Technology Data Exchange (ETDEWEB)

    Lopes, E.M., E-mail: eldermantovani@yahoo.com.b [Departamento de Fisica, Universidade Estadual de Londrina, CP 6001, CEP 86051-970 Londrina, Parana (Brazil); Duarte, J.L.; Pocas, L.C.; Dias, I.F.L.; Laureto, E. [Departamento de Fisica, Universidade Estadual de Londrina, CP 6001, CEP 86051-970 Londrina, Parana (Brazil); Quivy, A.A.; Lamas, T.E. [Laboratorio de Novos Materiais Semicondutores, Instituto de Fisica, Universidade de Sao Paulo, CP 66318, CEP 05315-970 Sao Paulo (Brazil)

    2010-03-15

    In this work, we present a detailed study on the optical properties of two GaAs/Al{sub 0.35}Ga{sub 0.65}As coupled double quantum wells (CDQWs) with inter-well barriers of different thicknesses, by using photoluminescence (PL) spectroscopy. The two CDQWs were grown in a single sample, assuring very similar experimental conditions for measurements of both. The PL spectrum of each CDQW exhibits two recombination channels which can be accurately identified as the excitonic e{sub 1}-hh{sub 1} transitions originated from CDQWs of different effective dimensions. The PL spectra characteristics and the behavior of the emissions as a function of temperature and excitation power are interpreted in the scenario of the bimodal interface roughness model, taking into account the exciton migration between the two regions considered in this model and the difference in the potential fluctuation levels between those two regions. The details of the PL spectra behavior as a function of excitation power are explained in terms of the competition between the band gap renormalization (BGR) and the potential fluctuation effects. The results obtained for the two CDQWs, which have different degrees of potential fluctuation, are also compared and discussed.

  8. Optical, Electrical and Magnetic Studies of Pi-Conjugated Organic Semiconductor Systems

    Energy Technology Data Exchange (ETDEWEB)

    Vardeny, Zeev Valentine [Univ. of Utah, Salt Lake City, UT (United States)

    2016-09-15

    Over the duration of this grant our group has studied the transient and cw optical response of various π-conjugated polymers, oligomers, single crystals, fullerene molecules and blends of organic donor-acceptor molecules. We have been also involved in complementary experiments such as magneto-optical studies and spin-physics. We have advanced the field of photophysics of these materials by providing information on their excited state energies and primodal and long-lived photoexcitations such as singlet excitons, triplet excitons, polaron-pairs, excimers and exciplexes. We also fabricated various organic optoelectronic devices such as organic light emitting diodes (OLED), electrochemical cells, organic diodes, organic spin-valves (OSV), and organic photovoltaic (OPV) solar cells. These devices benefited the society in terms of cheap and energy saving illumination, as well as harnessing the solar energy.

  9. Nonlinearity of the refractive index due to an excitonic molecule resonance state in CdS

    International Nuclear Information System (INIS)

    Baumert, R.; Broser, I.; Buschick, K.

    1986-01-01

    The authors report the observation of an intensity-dependent refractive-index nonlinearity in CdS due to a resonance state where an excitonic molecule is created by induced absorption of light. The refractive index n as a function of the incident laser photon energy E is measured directly by light refraction in thin crystal prisms. A renormalized dielectric function describes the measured n(E) spectra well. This strong refractive-index nonlinearity is well suited to produce an optical bistability and to further strengthen the evidence of CdS to be an important material for laser-induced dynamic gratings

  10. Absorption coefficients for interband optical transitions in a strained InAs1−xPx/InP quantum wire

    International Nuclear Information System (INIS)

    Saravanan, S.; John Peter, A.; Lee, Chang Woo

    2014-01-01

    Excitons confined in an InAs 1−x P x /InP (x=0.2) quantum well wire are studied in the presence of magnetic field strength. Numerical calculations are carried out using variational approach within the single band effective mass approximation. The compressive strain contribution to the confinement potential is included throughout the calculations. The energy difference of the ground and the first excited state is investigated in the influence of magnetic field strength taking into account the geometrical confinement effect. The magnetic field induced optical band as a function of wire radius is investigated in the InAs 0.8 P 0.2 /InP quantum well wire. The valence-band anisotropy is included in our theoretical model by employing different hole masses in different spatial directions. The optical gain as a function of incident photon energy is computed in the presence of magnetic field strength. The corresponding 1.55 μm wavelength is achieved for 40 Å InAs 0.8 P 0.2 /InP quantum well wire. We hope that the results could be used for the potential applications in fiber optic communications. -- Highlights: • Magnetic field induced excitons confined in a InAs 1−x P x /InP (x=0.2) quantum well wire are studied. • The compressive strain is included throughout the calculations. • The energy difference of the ground and the first excited state is investigated in the presence of magnetic field strength. • The magnetic field induced optical band with the geometrical confinement is studied. • The optical gain with the photon energy is computed in the presence of magnetic field strength

  11. Exciton localization-delocalization transition in an extended dendrimer

    Energy Technology Data Exchange (ETDEWEB)

    Pouthier, Vincent, E-mail: vincent.pouthier@univ-fcomte.fr [Institut UTINAM, Université de Franche-Comté, CNRS UMR 6213, 25030 Besançon Cedex (France)

    2013-12-21

    Exciton-mediated quantum state transfer between the periphery and the core of an extended dendrimer is investigated numerically. By mapping the dynamics onto that of a linear chain, it is shown that a localization-delocalization transition arises for a critical value of the generation number G{sub c} ≈ 5. This transition originates in the quantum interferences experienced by the excitonic wave due to the multiple scatterings that arise each time the wave tunnels from one generation to another. These results suggest that only small-size dendrimers could be used for designing an efficient quantum communication protocol.

  12. Exciton localization-delocalization transition in an extended dendrimer

    International Nuclear Information System (INIS)

    Pouthier, Vincent

    2013-01-01

    Exciton-mediated quantum state transfer between the periphery and the core of an extended dendrimer is investigated numerically. By mapping the dynamics onto that of a linear chain, it is shown that a localization-delocalization transition arises for a critical value of the generation number G c ≈ 5. This transition originates in the quantum interferences experienced by the excitonic wave due to the multiple scatterings that arise each time the wave tunnels from one generation to another. These results suggest that only small-size dendrimers could be used for designing an efficient quantum communication protocol

  13. Intrinsic homogeneous linewidth and broadening mechanisms of excitons in monolayer transition metal dichalcogenides

    KAUST Repository

    Moody, Galan; Kavir Dass, Chandriker; Hao, Kai; Chen, Chang-Hsiao; Li, Lain-Jong; Singh, Akshay; Tran, Kha; Clark, Genevieve; Xu, Xiaodong; Berghä user, Gunnar; Malic, Ermin; Knorr, Andreas; Li, Xiaoqin

    2015-01-01

    unknown property of valley excitons in these materials is the intrinsic homogeneous linewidth, which reflects irreversible quantum dissipation arising from system (exciton) and bath (vacuum and other quasiparticles) interactions and determines

  14. A Comparison Between Magnetic Field Effects in Excitonic and Exciplex Organic Light-Emitting Diodes

    Science.gov (United States)

    Sahin Tiras, Kevser; Wang, Yifei; Harmon, Nicholas J.; Wohlgenannt, Markus; Flatte, Michael E.

    In flat-panel displays and lighting applications, organic light emitting diodes (OLEDs) have been widely used because of their efficient light emission, low-cost manufacturing and flexibility. The electrons and holes injected from the anode and cathode, respectively, form a tightly bound exciton as they meet at a molecule in organic layer. Excitons occur as spin singlets or triplets and the ratio between singlet and triplet excitons formed is 1:3 based on spin degeneracy. The internal quantum efficiency (IQE) of fluorescent-based OLEDs is limited 25% because only singlet excitons contribute the light emission. To overcome this limitation, thermally activated delayed fluorescent (TADF) materials have been introduced in the field of OLEDs. The exchange splitting between the singlet and triplet states of two-component exciplex systems is comparable to the thermal energy in TADF materials, whereas it is usually much larger in excitons. Reverse intersystem crossing occurs from triplet to singlet exciplex state, and this improves the IQE. An applied small magnetic field can change the spin dynamics of recombination in TADF blends. In this study, magnetic field effects on both excitonic and exciplex OLEDs will be presented and comparison similarities and differences will be made.

  15. Exciton shelves for charge and energy transport in third-generation quantum-dot devices

    Science.gov (United States)

    Goodman, Samuel; Singh, Vivek; Noh, Hyunwoo; Casamada, Josep; Chatterjee, Anushree; Cha, Jennifer; Nagpal, Prashant

    2014-03-01

    Quantum dots are semiconductor nanocrystallites with size-dependent quantum-confined energy levels. While they have been intensively investigated to utilize hot-carriers for photovoltaic applications, to bridge the mismatch between incident solar photons and finite bandgap of semiconductor photocells, efficient charge or exciton transport in quantum-dot films has proven challenging. Here we show development of new coupled conjugated molecular wires with ``exciton shelves'', or different energy levels, matched with the multiple energy levels of quantum dots. Using single nanoparticle and ensemble device measurements we show successful extraction and transport of both bandedge and high-energy charge carriers, and energy transport of excitons. We demonstrate using measurements of electronic density of states, that careful matching of energy states of quantum-dot with molecular wires is important, and any mismatch can generate midgap states leading to charge recombination and reduced efficiency. Therefore, these exciton-shelves and quantum dots can lead to development of next-generation photovoltaic and photodetection devices using simultaneous transport of bandedge and hot-carriers or energy transport of excitons in these nanostructured solution-processed films.

  16. Phosphorescence as a probe of exciton formation and energy transfer in organic light emitting diodes

    International Nuclear Information System (INIS)

    Baldo, M.; Segal, M.

    2004-01-01

    The development of highly efficient phosphorescent molecules has approximately quadrupled the quantum efficiency of organic light emitting devices (OLEDs). By harnessing triplet as well as singlet excitons, efficient molecular phosphorescence has also enabled novel studies of exciton physics in organic semiconductors. In this review, we will summarize recent progress in understanding exciton formation and energy transfer using phosphorescent molecular probes. Particular emphasis is given to two topics of current interest: energy transfer in blue phosphorescent OLEDs, and quantifying the formation ratio of singlet to triplet excitons in small-molecular weight materials and polymers. (orig.)

  17. Plasmonic Structure Enhanced Exciton Generation at the Interface between the Perovskite Absorber and Copper Nanoparticles

    Science.gov (United States)

    Lin, Kuen-Feng; Chiang, Chien-Hung; Wu, Chun-Guey

    2014-01-01

    The refractive index and extinction coefficient of a triiodide perovskite absorber (TPA) were obtained by fitting the transmittance spectra of TPA/PEDOT:PSS/ITO/glass using the transfer matrix method. Cu nanoplasmonic structures were designed to enhance the exciton generation in the TPA and to simultaneously reduce the film thickness of the TPA. Excitons were effectively generated at the interface between TPA and Cu nanoparticles, as observed through the 3D finite-difference time-domain method. The exciton distribution is advantageous for the exciton dissociation and carrier transport. PMID:25295290

  18. Near-infrared magneto-optical study of excitonic states in single-walled carbon nanotubes under ultra-high magnetic fields

    International Nuclear Information System (INIS)

    Yokoi, H; Effendi, Mukhtar; Minami, N; Takeyama, S

    2011-01-01

    Singlet excitonic states at the first subband-edge in single-walled carbon nanotubes (SWCNTs) have been studied through near-infrared magneto-absorption spectroscopy under magnetic fields to 105.9 T. Well-resolved absorption spectra of stretch-aligned SWCNT(CoMoCAT)-gelatin films were obtained above 100 T. By the application of magnetic fields in parallel to the alignment of SWCNTs, peak shift toward the lower energy was observed for (8, 4) and (7, 6) tubes and the opposite behavior was observed for (7, 5) and (6, 5) tubes. Above 28.8 T, new peaks emerged at the higher energy side of the peak for the (8, 4) and (7, 6) tubes, and at the lower energy side of the peaks for the (7, 5) and (6, 5) tubes. The magnetic splitting between the existing peak and the new peak was symmetric for every tube, which is in line with the energy splitting due to the Aharonov-Bohm effect. Judging from the energetic positions where the new peaks emerged, the singlet dark excitonic state locates at the lower energy than the singlet bright one in the (7, 5) and (6, 5) tubes while it is suggested strongly that the bright one locates at the lower energy in the (8, 4) and (7, 6) tubes.

  19. Optical spectroscopy of two-dimensional layered (C(6)H(5)C(2)H(4)-NH(3))(2)-PbI(4) perovskite.

    Science.gov (United States)

    Gauthron, K; Lauret, J-S; Doyennette, L; Lanty, G; Al Choueiry, A; Zhang, S J; Brehier, A; Largeau, L; Mauguin, O; Bloch, J; Deleporte, E

    2010-03-15

    We report on optical spectroscopy (photoluminescence and photoluminescence excitation) on two-dimensional self-organized layers of (C(6)H(5)C(2)H(4)-NH(3))(2)-PbI(4) perovskite. Temperature and excitation power dependance of the optical spectra gives a new insight into the excitonic and the phononic properties of this hybrid organic/inorganic semiconductor. In particular, exciton-phonon interaction is found to be more than one order of magnitude higher than in GaAs QWs. As a result, photoluminescence emission lines have to be interpreted in the framework of a polaron model.

  20. Hydrostatic stress dependence of the exciton-phonon coupled states in cylindrical quantum dots

    International Nuclear Information System (INIS)

    El Moussaouy, A.; Bria, D.; Nougaoui, A.

    2005-01-01

    We investigate theoretically the effects of compressive stress on the binding energy of an exciton in a cylindrical quantum dot (QD) using a variational procedure within the effective mass approximation. The stress was applied in the z direction and the interaction between the charge carriers (electron and hole) and confined longitudinal optical (LO) phonon modes was taken into account. Specific applications of these results are given for GaAs QDs embedded in a Ga 1-x Al x As semiconductor. The result shows that the binding energy and the polaronic correction increases linearly with increasing stress. Moreover, we obtain the binding energy and the polaronic contribution in the limit in which the QD turns into a quantum well