Nelson, Heidi D; Bradshaw, Liam R; Barrows, Charles J; Vlaskin, Vladimir A; Gamelin, Daniel R
2015-11-24
Spontaneous magnetization is observed at zero magnetic field in photoexcited colloidal Cd(1-x)Mn(x)Se (x = 0.13) quantum dots (QDs) prepared by diffusion doping, reflecting strong Mn(2+)-exciton exchange coupling. The picosecond dynamics of this phenomenon, known as an excitonic magnetic polaron (EMP), are examined using a combination of time-resolved photoluminescence, magneto-photoluminescence, and Faraday rotation (TRFR) spectroscopies, in conjunction with continuous-wave absorption, magnetic circular dichroism (MCD), and magnetic circularly polarized photoluminescence (MCPL) spectroscopies. The data indicate that EMPs form with random magnetization orientations at zero external field, but their formation can be directed by an external magnetic field. After formation, however, external magnetic fields are unable to reorient the EMPs within the luminescence lifetime, implicating anisotropy in the EMP potential-energy surfaces. TRFR measurements in a transverse magnetic field reveal rapid (<5 ps) spin transfer from excitons to Mn(2+) followed by coherent EMP precession at the Mn(2+) Larmor frequency for over a nanosecond. A dynamical TRFR phase inversion is observed during EMP formation attributed to the large shifts in excitonic absorption energies during spontaneous magnetization. Partial optical orientation of the EMPs by resonant circularly polarized photoexcitation is also demonstrated. Collectively, these results highlight the extraordinary physical properties of colloidal diffusion-doped Cd(1-x)Mn(x)Se QDs that result from their unique combination of strong quantum confinement, large Mn(2+) concentrations, and relatively narrow size distributions. The insights gained from these measurements advance our understanding of spin dynamics and magnetic exchange in colloidal doped semiconductor nanostructures, with potential ramifications for future spin-based information technologies.
Gnatenko, Yu. P. Bukivskij, P. M.; Piryatinski, Yu. P.
2014-04-07
We have investigated dynamics of different localized exciton magnetic polarons (LEMPs) in Cd{sub 0.70}Mn{sub 0.30}Te spin glass (SG) compound below the freezing temperature T{sub f} in the crystal regions, where various microscopic magnetic spin states (MMSSs), namely, “loose” spins, finite, and infinite clusters, are formed. It was shown that there is a broad distribution of the LEMPs lifetimes. The presence of the long-lived LEMPs is caused by the admixture of the optically active bright exciton states to the dark exciton states, i.e., the “brightening” of the dark LEMPs which exist along with the bright LEMPs. The lifetimes of the dark LEMPs correspond to hundreds of nanoseconds. It was found that the time decay of photoluminescence band intensity is approximated by the sum of two functions: a single exponential function and the Kohlrausch–Williams–Watts stretched exponential function. The stretched exponential function describes the recombination processes of the LEMPs formed in the crystal regions of the finite clusters as well as the infinite cluster. This reflects the appearance of spatially heterogeneous dynamics in Cd{sub 0.70}Mn{sub 0.30}Te SG compound below T{sub f} which is due to the disorder in the spin distribution caused by the formation of different MMSSs.
Magnetic polaron formation and exciton spin relaxation in single Cd1-xMnxTe quantum dots
NASA Astrophysics Data System (ADS)
Kłopotowski, Ł.; Cywiński, Ł.; Wojnar, P.; Voliotis, V.; Fronc, K.; Kazimierczuk, T.; Golnik, A.; Ravaro, M.; Grousson, R.; Karczewski, G.; Wojtowicz, T.
2011-02-01
We study the formation dynamics of a spontaneous ferromagnetic order in single self-assembled Cd1-xMnxTe quantum dots (QDs). By measuring time-resolved photoluminescence, we determine the formation times for QDs with Mn ion contents x varying from 0.01 to 0.2. At low x these times are orders of magnitude longer than exciton spin relaxation times evaluated from the decay of photoluminescence circular polarization. This allows us to conclude that the direction of the spontaneous magnetization is determined by a momentary Mn spin fluctuation rather than resulting from an optical orientation. At higher x, the formation times are of the same order of magnitude as found in previous studies on higher-dimensional systems. We also find that the exciton spin relaxation accelerates with increasing Mn concentration.
Optical dynamics of exciton and polaron formation in molecular aggregates
NASA Astrophysics Data System (ADS)
de Boer, Steven; Wiersma, Douwe A.
1989-03-01
Results of femtosecond accumulated photon echo, picosecond pump-probe and fluorescence lifetime measurements are reported on aggregates of the dyes pseudoisocyanine (PIC) and substituted thiapyrylium (TPY), embedded in a polycarbonate matrix. It is concluded that in the PIC aggregate, delocalized excitations (excitons) are formed, which are weakly coupled to the aggregate's nuclear frame. In the TPY aggregate, excitons are also initially formed, but through strong local electron-phonon coupling these excitons are not stable and decay into polarons, which become trapped. It is suggested that the nature of the excitations in aggregates crucially depends on the change of electron density distribution upon optical excitation. When this change is large, as revealed by a large change of dipole moment, polarons will be formed. In the other limit of a small change of dipole moment on optical excitation, excitons with an enhanced radiative lifetime are formed, which coherently propagate over that part of the aggregate where the molecules are electronically strongly coupled. The relevance of these findings towards energy transport in photo-biological systems is also discussed.
Polaronic trapping in magnetic semiconductors
NASA Astrophysics Data System (ADS)
Raebiger, Hannes
2012-02-01
GaN doped with iron is an interesting candidate material for magnetic semiconductors, as p-d coupling between the localized Fe-d and extended N-p hole states is expected to facilitate long-range ferromagnetic alignment of the Fe spins [1]. This picture of extended states in GaN:Fe, however, falls apart due to a polaronic localization of the hole carriers nearby the Fe impurities. To elucidate the carrier localization in GaN:Fe and related iron doped III-V semiconductors, I present a systematic study using self-interaction corrected density-functional calculations [2]. These calculations predict three distinct scenarios. (i) Some systems do sustain extended host-like hole states, (ii) some exhibit polaronic trapping, (iii) and some exhibit carrier trapping at Fe-d orbitals. These behaviors are described in detail to give an insight as to how to distinguish them experimentally. I thank T. Fujita, C. Echeverria-Arrondo, and A. Ayuela for their collaboration.[4pt] [1] T. Dietl et al, Science, 287, 1019 (2000).[0pt] [2] S. Lany and A. Zunger, Phys. Rev. B, 80, 085202 (2009).
NASA Astrophysics Data System (ADS)
Hershey, Kyle W.; Holmes, Russell J.
2016-11-01
Phosphorescent organic light-emitting devices (OLEDs) can suffer a significant reduction in device efficiency under high current density excitation. This steady-state efficiency roll-off is frequently modeled by including losses from exciton-exciton and exciton-polaron quenching. Despite success in modeling the steady-state efficiency roll-off, the corresponding transient electroluminescence behavior has not been modeled as effectively using the same quenching processes. In this work, both the steady-state and transient electroluminescence behavior of phosphorescent OLEDs based on tris[2-phenylpyridinato-C2,N]Iridium(III) (Ir(ppy)3) are successfully reproduced by considering a dynamic polaron population. Within this model, polarons are able to either form excitons or leak through the device emissive layer, reducing the overall efficiency. This formalism permits a natural and rigorous connection between exciton and polaron dynamics and device charge balance, with the charge balance cast as the efficiency of exciton formation. The full dynamics model reproduces both the rise and decay of transient electroluminescence, as well as the full dependence of the external quantum efficiency on current density. Fit parameters are independently verified using separate studies of transient and steady-state photoluminescence. The model provides a complete picture for the dynamics present during the electrical operation of phosphorescent OLEDs, while also offering a direct route to elucidate exciton formation.
Energy Migration in Organic Thin Films--From Excitons to Polarons
NASA Astrophysics Data System (ADS)
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.
Magnetic polaron on dangling-bond spins in CdSe colloidal nanocrystals.
Biadala, Louis; Shornikova, Elena V; Rodina, Anna V; Yakovlev, Dmitri R; Siebers, Benjamin; Aubert, Tangi; Nasilowski, Michel; Hens, Zeger; Dubertret, Benoit; Efros, Alexander L; Bayer, Manfred
2017-03-13
Non-magnetic colloidal nanostructures can demonstrate magnetic properties typical for diluted magnetic semiconductors because the spins of dangling bonds at their surface can act as the localized spins of magnetic ions. Here we report the observation of dangling-bond magnetic polarons (DBMPs) in 2.8-nm diameter CdSe colloidal nanocrystals (NCs). The DBMP binding energy of 7 meV is measured from the spectral shift of the emission lines under selective laser excitation. The polaron formation at low temperatures occurs by optical orientation of the dangling-bond spins (DBSs) that result from dangling-bond-assisted radiative recombination of spin-forbidden dark excitons. Modelling of the temperature dependence of the DBMP-binding energy and emission intensity shows that the DBMP is composed of a dark exciton and about 60 DBSs. The exchange integral of one DBS with the electron confined in the NC is ∼0.12 meV.
NASA Astrophysics Data System (ADS)
Udal'tsov, Alexander V.
2016-12-01
Assemblies consisting of protonated meso-tetraphenylporphine (TPP) dimers and water have been investigated by UV-vis and infrared (IR) spectroscopy and by atomic force microscopy (AFM) in thin layers. Features of electronic absorption spectra of the assemblies are interpreted in terms of hole polaron combined with exciton theory using quantum well with parameters obtained from the dimer structure. It appears to be hole polaron moving defines kinetic energy of polaronic exciton confined in a quantum well when the electron absorbs photon. Hole polaron characteristics such as polaron self-energy, energy of Frank-Condon transitions, and radius of hole polaron moving through water are found to be 1.38 eV, 0.2445 eV, and 0.246 Å, respectively. A doublet at 1944, 1960 cm-1 (0.2412, 0.2432 eV) observed in IR spectra matches the energy of Frank-Condon transitions. Excitation energies estimated using molecular parameters for polaronic excitons in pure water and in the TPP dimers are found in a good agreement with the experimental data.
Photoinduced giant magnetic polarons in EuTe
NASA Astrophysics Data System (ADS)
Henriques, A. B.; Naupa, A. R.; Usachev, P. A.; Pavlov, V. V.; Rappl, P. H. O.; Abramof, E.
2017-01-01
Photoinduced magnetic polarons in EuTe, with a magnetic moment of several hundred Bohr magnetons, were investigated as a function of pump intensity and temperature by pump-probe Faraday rotation. The quantum efficiency for optical generation of magnetic polarons is found to be 0.09. The pump-intensity dependence of the photoinduced Faraday rotation shows a sublinear increase, from which we deduce that the population of photoexcited polarons is limited by a maximum value of 4.5 ×1015cm-3 . This is four orders of magnitude less than the concentration of polarons that would completely fill the crystal, which suggests that the photoexcited polarons are anchored by defects. In addition to the generation of polarons, at high pump densities the modulated pump light also causes a small alternating heating of the illuminated region. The temperature dependence of the polaron magnetic moment is well described by the Curie-Weiss law. Above 100 K, polarons are thermally quenched with an activation energy of 11 meV.
Excitonic-type polaron states: photoluminescence in SBN and in other ferroelectric oxides
NASA Astrophysics Data System (ADS)
Vikhnin, V. S.; Kislova, I.; Kutsenko, A. B.; Kapphan, S. E.
2002-07-01
A theoretical model for two characteristic photoluminescence (PL) bands in SBN, 'green luminescence' and 'red luminescence' is proposed on the basis of the extended photoluminescence experiments in SBN:Cr, and also in SBN:Ce and in nominally pure SBN systems under different conditions. While the RL-band is suggested to be connected with charge transfer vibronic exciton (CTVE) clusters induced by Cr3+ impurities in the Nb-sites, the GL- band is connected with Nb4+ electronic polarons in a new, charge transfer excited states. Here Nb4+ centers are the cores of the CTVE clusters induced by these charged scores. The PL mechanism is the in-cluster CTVE recombination for both bands under discussion. But the CTVE states are quasi-resonantly mixed here with 4T2 states of the Cr3+ core in the RL-band case, and with 5s-states of the Nb4+ core in the GL-band case. The role of excitonic polarons of CTVE nature is also discussed in connection with 'green' luminescence origin in KTaO3 and KNbO3 crystals.
NASA Astrophysics Data System (ADS)
Kotomin, E. A.; Eglitis, R. I.; Borstel, G.
2000-09-01
Quantum chemical calculations using the intermediate neglect of the differential overlap (INDO) method, combined with the large unit cell periodic model argue for an existence of the self-trapped electrons in KNbO3 and KTaO3 perovskite crystals. An electron in the ground state occupies predominantly t2g orbital of a Nb4+ ion. Its orbital degeneracy is lifted by a combination of the breathing and Jahn-Teller modes where four nearest equatorial O atoms are displaced outwards and two oxygens shift inwards along the z axis. Triplet exciton is shown to be in a good approximation of a pair of nearest Jahn-Teller electron and hole polarons (a bipolaron) which is very likely responsible for the `green' luminescence observed in these crystals.
Two-dimensional polaron in a magnetic field
NASA Astrophysics Data System (ADS)
Xiaoguang, Wu; Peeters, F. M.; Devreese, J. T.
1985-12-01
The ground-state energy of a Fröhlich optical polaron confined to two dimensions, placed in a perpendicular magnetic field is calculated within the Feynman path-integral approach. The Feynman-model mass, the magnetization and the susceptibility are calculated as a function of the magnetic field strength for different values of the electron-phonon coupling. We find that within the generalized Feynman approximation the polaron exhibits a discontinuous transition from a dressed state to a stripped state if the electron-phonon constant α is larger than 1.60. For α<1.60, the transition occurs continuously with increasing magnetic field.
Liu, Jin; Adamska, Lyudmyla; Doorn, Stephen K.; Tretiak, Sergei
2015-05-14
Conformational structure and the electronic properties of various electronic excitations in cycloparaphenylenes (CPPs) are calculated using hybrid Density Functional Theory (DFT). The results demonstrate that wavefunctions of singlet and triplet excitons as well as the positive and negative polarons remain fully delocalized in CPPs. In contrast, these excitations in larger CPP molecules become localized on several phenyl rings, which are locally planarized, while the undeformed ground state geometry is preserved on the rest of the hoop. As evidenced by the measurements of bond-length alternation and dihedral angles, localized regions show stronger hybridization between neighboring bonds and thus enhanced electronic communication. This effect is even more significant in the smaller hoops, where phenyl rings have strong quinoid character in the ground state. Thus, upon excitation, electron–phonon coupling leads to the self-trapping of the electronic wavefunction and release of energy from fractions of an eV up to two eVs, depending on the type of excitation and the size of the hoop. The impact of such localization on electronic and optical properties of CPPs is systematically investigated and compared with the available experimental measurements.
Liu, Jin; Adamska, Lyudmyla; Doorn, Stephen K.; ...
2015-05-14
Conformational structure and the electronic properties of various electronic excitations in cycloparaphenylenes (CPPs) are calculated using hybrid Density Functional Theory (DFT). The results demonstrate that wavefunctions of singlet and triplet excitons as well as the positive and negative polarons remain fully delocalized in CPPs. In contrast, these excitations in larger CPP molecules become localized on several phenyl rings, which are locally planarized, while the undeformed ground state geometry is preserved on the rest of the hoop. As evidenced by the measurements of bond-length alternation and dihedral angles, localized regions show stronger hybridization between neighboring bonds and thus enhanced electronic communication.more » This effect is even more significant in the smaller hoops, where phenyl rings have strong quinoid character in the ground state. Thus, upon excitation, electron–phonon coupling leads to the self-trapping of the electronic wavefunction and release of energy from fractions of an eV up to two eVs, depending on the type of excitation and the size of the hoop. The impact of such localization on electronic and optical properties of CPPs is systematically investigated and compared with the available experimental measurements.« less
Effects of sp-d exchange on a bound polaron and the g-factor of the exciton in a GaMnAs quantum dot
NASA Astrophysics Data System (ADS)
Lalitha, D.; John Peter, A.; Yoo, Chang Kyoo
2013-08-01
Magneto bound polaron in a GaMnAs/Ga0.6Al0.4As quantum dot is investigated with the inclusion of exchange interaction effects due to Mn alloy content and the geometrical confinement. The exciton binding energy and the optical transition energy are computed as functions of dot radius and the magnetic field strength for a fixed Mn alloy content (x = 0.02) in a GaMnAs quantum dot. Numerical calculations are performed using variational method within a single band effective mass approximation. The spin polaronic energy of the heavy hole exciton is studied with the spatial confinement using a mean field theory in the presence of magnetic field strength. The magnetization as a function of dot radius is investigated in a GaMnAs/Ga0.6Al0.4As quantum dot. The magnetic field induced size dependence of g-factor is studied. The effective g-factor of conduction (valence) band electron (hole) is obtained in the GaMnAs quantum dot. The results bring out that (i) the geometrical dependence on sp-d exchange interaction in the GaMnAs/Ga0.6Al0.4As quantum dot has great influence with the magnetic field strength, (ii) the Landé factor is more sensitive if the geometrical confinement effect is included and (iii) the value of g-factor increases when the magnetic field strength is enhanced for all the dot radii. Our results are in good agreement with the other investigators.
Experimental manifestations of the Nb4+-O- polaronic excitons in KTa0.988Nb0.012O3
NASA Astrophysics Data System (ADS)
Yusupov, R. V.; Gracheva, I. N.; Rodionov, A. A.; Syrnikov, P. P.; Gubaev, A. I.; Dejneka, A.; Jastrabik, L.; Trepakov, V. A.; Salakhov, M. Kh.
2011-11-01
The formation of the photopolaronic excitons in ABO3 perovskite-type oxides has been detected experimentally by means of the photoinduced electron paramagnetic resonance (EPR) studies of KTa0.988Nb0.012O3 crystals. The corresponding microwave x-band spectrum at T< 10 K consists of a narrow, nearly isotropic signal located at g ˜ 2 and a strongly anisotropic component. The first signal, which has a rich structure due to hyperfine interactions with the lattice nuclei, is attributed to the single trapped charge carriers: the electrons and/or the holes. The anisotropic spectrum is caused by the axial centers oriented along the C4 pseudocubic principal crystalline axes. The spectrum angular dependence can be described well by an axial center with S = 1, g∥ = 0.82, g⊥ = 0.52, and D = 0.44 cm-1. The anisotropic spectrum is attributed to the Nb4+-O- polaronic excitons. The temperature dependence of the anisotropic component is characterized by two activation energies: the internal dynamics activation Ea1 = 3.7 ± 0.5 meV, which makes the EPR spectrum unobservable above 10 K, and the destruction energy Ea2 = 52 ± 4 meV. By comparing the anisotropic photo-EPR spectrum and the photoinduced optical absorption temperature dependencies, we found that the Nb4+-O- polaronic excitons also manifested themselves via the wide absorption band at ˜0.7 eV arising under ultraviolet light excitation in the weakly concentrated KTaO3:Nb crystals.
Magnetic-Polaron-Induced Enhancement of Surface Raman Scattering
Shao, Qi; Liao, Fan; Ruotolo, Antonio
2016-01-01
The studies of the effects of magnetic field on surface enhanced Raman scattering (SERS) have been so far limited to the case of ferromagnetic/noble-metal, core/shell nano-particles, where the influence was always found to be negative. In this work, we investigate the influence of magnetic field on a diluted magnetic semiconductor/metal SERS system. Guided by three dimensional finite-difference time-domain simulations, a high efficient SERS substrate was obtained by diluting Mn into Au-capped ZnO, which results in an increase of the dielectric constant and, therefore, an enhancement of Raman signals. More remarkably, an increase of intensities as well as a reduction of the relative standard deviation (RSD) of Raman signals have been observed as a function of the external magnetic strength. We ascribe these positive influences to magnetic-field induced nucleation of bound magnetic polarons in the Mn doped ZnO. The combination of diluted magnetic semiconductors and SERS may open a new avenue for future magneto-optical applications. PMID:26754049
Magnetic-polaron-induced colossal magnetocapacitance in CdCr2S4
NASA Astrophysics Data System (ADS)
Xie, Y. M.; Yang, Z. R.; Zhang, Z. T.; Yin, L. H.; Chen, X. L.; Song, W. H.; Sun, Y. P.; Zhou, S. Q.; Tong, W.; Zhang, Y. H.
2013-10-01
The origin of colossal magnetoresistance and colossal magnetocapacitance in a CdCr2S4 system was investigated. Thermoelectric-power and electronic spin resonance spectra reveal that the magnetic polaron is responsible for the colossal magnetoresistance in the n-type sample. The existence of magnetic polarons in the paramagnetic insulting matrix forms an intrinsic Maxwell-Wagner system, leading to the appearance of colossal magnetocapacitance. Being consistent with the evolution of magnetic polarons upon cooling, the Maxwell-Wagner system is valid around insulator-metal transition, where the resistance derived from impedance spectroscopy matches perfectly with DC resistance.
Magnetic hard gap due to bound magnetic polarons in the localized regime
NASA Astrophysics Data System (ADS)
Rimal, Gaurab; Tang, Jinke
2017-02-01
We investigate the low temperature electron transport properties of manganese doped lead sulfide films. The system shows variable range hopping at low temperatures that crosses over into an activation regime at even lower temperatures. This crossover is destroyed by an applied magnetic field which suggests a magnetic origin of the hard gap, associated with bound magnetic polarons. Even though the gap forms around the superconducting transition temperature of lead, we do not find evidence of this being due to insulator-superconductor transition. Comparison with undoped PbS films, which do not show the activated transport behavior, suggests that bound magnetic polarons create the hard gap in the system that can be closed by magnetic fields.
Magnetic hard gap due to bound magnetic polarons in the localized regime
Rimal, Gaurab; Tang, Jinke
2017-01-01
We investigate the low temperature electron transport properties of manganese doped lead sulfide films. The system shows variable range hopping at low temperatures that crosses over into an activation regime at even lower temperatures. This crossover is destroyed by an applied magnetic field which suggests a magnetic origin of the hard gap, associated with bound magnetic polarons. Even though the gap forms around the superconducting transition temperature of lead, we do not find evidence of this being due to insulator-superconductor transition. Comparison with undoped PbS films, which do not show the activated transport behavior, suggests that bound magnetic polarons create the hard gap in the system that can be closed by magnetic fields. PMID:28176857
A magnetic polaron model for the enhanced Curie temperature of EuO(1-x).
Liu, Pan; Tang, Jinke
2013-03-27
The investigation of a series of oxygen-deficient EuO thin films provided strong evidence that the doped electrons form magnetic polarons with the nearby Eu2+ 4f spins; this is responsible for the enhanced Curie temperature observed near 140 K. Unlike in the previous magnetic polaron models proposed for the metal-to-insulator transition in EuO, the exchange coupling J between the doped electron and its neighboring 4f spins is antiferromagnetic. The model explains satisfactorily the fact that the ordering temperature of the magnetic polarons occurs at ~140 K, independently of the oxygen vacancy concentration, and the contradiction that electron doping increases T(c) and yet reduces the red shift in the optical absorption. The magnetic polarons are coupled antiferromagnetically to the Eu2+ local moments that are ordered in the Heisenberg ferromagnet below 69 K. This coupling was observable in the vicinity of 69 K. We discuss how, with increasing concentration of the oxygen vacancies, their behaviors evolve from those of isolated superparamagnetic polarons to those of percolating magnetic polarons with a finite coercivity.
Spin-Induced Optical Phenomena in Diluted Magnetic Semiconductors
NASA Astrophysics Data System (ADS)
Takeyama, Shojiro
The following sections are included: * INTRODUCTION * GENERAL FEATURES * Materials * Crystal Structures * Band Structure at ěc{k}≃ 0 * sp-d Exchange Interaction * Magnetic Properties and Parameters * Magnetization Steps due to Nearest-Neighbor Spin Pairs * The Physical Origin of the sp-d Exchange Constants * OPTICAL RESPONSE OF THE LOW-DIMENSIONAL DMSs * Anisotropy of the Zeeman Effect in Two-Dimensional DMSs * Magneto-Optical Method of Interface Characterization * MAGNETIC POLARONS * Bound Magnetic Polarons * Free Magnetic Polarons * OPTICAL OBSERVATION OF MAGNETIC POLARONS * A Selective Excitation Photoluminescence Study * Optical Survey of Free Magnetic Polarons * Two-Dimensional Exciton Free Magnetic Polarons * SUMMARY * REFERENCES
Transport of indirect excitons in high magnetic fields
NASA Astrophysics Data System (ADS)
Kuznetsova, Y. Y.; Dorow, C. J.; Calman, E. V.; Butov, L. V.; Wilkes, J.; Muljarov, E. A.; Campman, K. L.; Gossard, A. C.
2017-03-01
We present spatially and spectrally resolved photoluminescence measurements of indirect excitons in high magnetic fields. Long indirect exciton lifetimes give the opportunity to measure magnetoexciton transport by optical imaging. Indirect excitons formed from electrons and holes at zeroth Landau levels (0e-0h indirect magnetoexcitons) travel over large distances and form a ring emission pattern around the excitation spot. In contrast, the spatial profiles of 1e-1h and 2e-2h indirect magnetoexciton emission closely follow the laser excitation profile. The 0e-0h indirect magnetoexciton transport distance reduces with increasing magnetic field. These effects are explained in terms of magnetoexciton energy relaxation and effective mass enhancement.
Excitonic magnetism in d6 perovskites
NASA Astrophysics Data System (ADS)
Afonso, J. Fernández; Kuneš, J.
2017-03-01
We use the LDA+U method to study the possibility of exciton condensation in perovskites of transition metals with the d6 electronic configuration such as LaCoO3. For realistic interaction parameters we find several distinct solutions exhibiting a spin-triplet exciton condensate, which gives rise to a local spin density distribution while the ordered moments are vanishingly small. Rhombohedral distortion from the ideal cubic structure suppresses the ordered state, contrary to the spin-orbit coupling which enhances the excitonic condensation energy. We explain the trends observed in the numerical simulations with the help of a simplified strong-coupling model. Our results indicate that LaCoO3 is close to the excitonic instability and suggest ways how to achieve the exciton condensation.
Anomalous magnetization of a carbon nanotube as an excitonic insulator
NASA Astrophysics Data System (ADS)
Rontani, Massimo
2014-11-01
We show theoretically that an undoped carbon nanotube might be an excitonic insulator—the long-sought phase of matter proposed by Keldysh, Kohn, and others fifty years ago. We predict that the condensation of triplet excitons, driven by intervalley exchange interaction, spontaneously occurs at equilibrium if the tube radius is sufficiently small. The signatures of exciton condensation are its sizable contributions to both the energy gap and the magnetic moment per electron. The increase of the gap might have already been measured, albeit with a different explanation [V. V. Deshpande, B. Chandra, R. Caldwell, D. S. Novikov, J. Hone, and M. Bockrath, Science 323, 106 (2009), 10.1126/science.1165799]. The enhancement of the quasiparticle magnetic moment is a pair-breaking effect that counteracts the weak paramagnetism of the ground-state condensate of excitons. This property could rationalize the anomalous magnitude of magnetic moments recently observed in different devices close to charge neutrality.
Electric and magnetic optical polaron in quantum dot—Part 1: strong coupling
NASA Astrophysics Data System (ADS)
Fotue, A. J.; Issofa, N.; Tiotsop, M.; Kenfack, S. C.; Tabue Djemmo, M. P.; Fotsin, H.; Fai, L. C.
2015-07-01
We investigated the influence of electric field and magnetic field on the ground state energy of polaron in spherical semiconductor quantum dot (QD) using a modified Lee Low Pines (LLP) method. The numerical results show the increase of the ground state energy with the increase of the electric field and the decreasing with the magnetic field. The modulation of the electric field, magnetic field and the confinement lengths lead to the control of the decoherence of the system.
Modeling of magnetic polaron properties in (Zn,Mn)Te quantum dots
NASA Astrophysics Data System (ADS)
Pientka, James; Barman, B.; Schweidenback, L.; Russ, A. H.; Tsai, Y.; Murphy, J. R.; Cartwright, A. N.; Zutic, I.; McCombe, B. D.; Petrou, A.; Chou, W.-C.; Fan, W. C.; Sellers, I. R.; Petukhov, A. G.; Oszwaldowski, R.
Magnetic polarons in (Zn,Mn)Te quantum dots (QD) show unconventional behavior. These structures exhibit a small red shift of the photoluminescence peak energy in the presence of a magnetic field B and they also have a weak dependence of the polaron energy EMP on temperature T and B. We attribute these properties to a large molecular field Bm that is proportional to the heavy holes spin density. We have calculated Bm using the QD diameter and height as adjustable parameters. Assuming hole localization, this calculation yields values of Bm >20 T. The assumption that the hole localization diameter can be smaller than the QD diameter is justified due to alloy and spin disorder scattering. Using the magnetic polaron free energy, we calculate EMP as function of T and B for a variety of Bm values. To get a weak dependence of EMP on T and Bwe must assume that the polaron temperature is higher than T. This work was supported by U.S. DOE BES, Award DE-SC0004890, NSF DMR-1305770 and U.S. ONR N000141310754.
Compensation of dipolar-exciton spin splitting in magnetic field
NASA Astrophysics Data System (ADS)
Gorbunov, A. V.; Timofeev, V. B.
2013-03-01
Magnetoluminescence of spatially indirect dipolar excitons in 25 nm GaAs/AlGaAs single quantum well collected within a lateral potential trap has been studied in Faraday geometry. The paramagnetic spin splitting of the luminescence line of the heavy-hole excitons in the trap centre is completely compensated at magnetic field below critical value ≈2 Т. The effect of spin splitting compensation is caused by the exchange interaction in dense exciton Bose gas which is in qualitative agreement with the existing theoretical concepts.
NASA Astrophysics Data System (ADS)
Peter, A. John; Zheng, Jin-Liang
2010-04-01
Theoretical investigations of spin polaron in a quantum well in the spin doping superlattice systems Cd1 - xin Mn1 - xout Te/Cd1 - xout Mnxout Te are presented in this paper. A variational procedure within the effective mass approximation is employed in the presence of magnetic held to calculate the donor ionization energy. Spin polaronic shifts are estimated using a mean held theory. The results show that the donor binding energy (i) Increases with the reduction in well sizes (ii) Decreases with the magnetic held is increased for a given well width (iii) Increases to a maximum value at 90 Å and then decreases as the size of the well increases beyond 90 Å and (iv) Spin polaronic shifts to the donor binding energy not only decrease in a magnetic held but also with the well width. The results are compared with the existing available literature.
Magnetic brightening of dark excitons in transitional metal dichalcogenides
NASA Astrophysics Data System (ADS)
Zhang, Xiao-Xiao; Lu, Zhengguang; Cao, Ting; Zhang, Fan; Hone, James; Louie, Steven G.; Li, Zhiqiang; Smirnov, Dmitry; Heinz, Tony
Transitional metal dichalcogenides (TMDC) in the MX2 (M = Mo, W, X = S, Se) family represent an excellent platform to study of excitonic effects. At monolayer thickness, these materials exhibit both direct band-gap character and enhanced excitonic interactions. Theoretical studies suggest that both the valence and conduction bands are split and exhibit spin polarized character at the K/K' valleys. The lowest energy band-edge excitons are predicted to have different spin configurations for different materials in this family. When the lowest lying exciton has parallel electron and hole spin, radiative decay is forbidden and the state is dark. Here we demonstrate that by applying an in-plane magnetic field we can perturb the exciton spin configuration and brighten this state, allowing it to undergo radiative decay. We identify such a brightened dark state by the emergence of a new emission peak lying below the absorption peak, with a strength growing with applied in-plane magnetic field. On the other hand, for monolayer MoSe2, where no low-lying dark state is expected, we do not see the growth of a new emission feature under application of an in-plane magnetic field. Our experimental findings are in agreement with the calculated properties of dark excitons based on GW plus Bethe-Salpeter equation approach
Magnetic polarons in type-II (Zn,Mn)Se/ZnTe quantum dots
NASA Astrophysics Data System (ADS)
Murphy, J. R.; Barman, B.; Tsai, Y.; Scrace, T.; Pientka, J. M.; Zutic, I.; McCombe, B. D.; Petrou, A.; Cartwright, A. N.; Chou, W. C.; Tsou, M. H.; Yang, C. S.; Sellers, I. R.; Oszwaldowski, R.; Petukhov, A. G.
2014-03-01
We have studied magnetic polaron formation dynamics in (Zn,Mn)Se/ZnTe quantum dots2 (QDs) using time-resolved photoluminescence (TRPL) spectroscopy. The emitted light was spectrally and temporally analyzed; the emission spectra were recorded as function of time delay (Δt) from the exciting laser pulse. The recombination time at T = 10 K in our samples is 2.3 ns. The peak energy of the emission red shifts with increasing Δt due to the lowering of the hole-Mn spin complex (magnetic polaron) energy. From this shift we determined the magnetic polaron formation energy (EMP) at T = 10 K to be 20 meV, which is half the value observed in the ZnSe/(Zn,Mn)Te system studied previously.3EMP decreases with increasing temperature, in contrast to the behavior of the ZnSe/(Zn,Mn)Te system3 in which EMP is temperature independent. These results are discussed in terms of a theoretical model. This work is supported by DOE-BES, ONR and NSF.
Magnetic edge-state excitons in zigzag graphene nanoribbons.
Yang, Li; Cohen, Marvin L; Louie, Steven G
2008-10-31
We present first-principles calculations of the optical properties of zigzag-edged graphene nanoribbons (ZGNRs) employing the GW-Bethe-Salpeter equation approach with the spin interaction included. Optical response of the ZGNRs is found to be dominated by magnetic edge-state-derived excitons with large binding energy. The absorption spectrum is composed of a characteristic series of exciton states, providing a possible signature for identifying the ZGNRs. The edge-state excitons are charge-transfer excitations with the excited electron and hole located on opposite edges; they moreover induce a spin transfer across the ribbon, resulting in a photoreduction of the magnetic ordering. These novel characteristics are potentially useful in the applications.
Zhang, Yingjie; Aziz, Hany
2016-06-08
The root causes of the differences in electroluminescence stability among phosphorescent organic light-emitting devices (PHOLEDs) utilizing different emitter guests are studied. The results show that the host material plays a more influential role in limiting device stability in comparison to the guest. During the operation of a PHOLED, the host undergoes aggregation as a result of interactions between the excitons and positive polarons. The rate of this aggregation is found to be the limiting factor for device lifetime and is influenced by the choice of the guest material and its concentration. Finally, it is shown that phase segregation between the host and the guest is an important aspect of the aggregation process. As a result of this segregation, energy transfer from the host to the guest becomes increasingly less efficient, resulting in the observed gradual loss in electroluminescence efficiency in the devices over time. The findings explain why PHOLEDs utilizing different guest materials but otherwise identical material systems can have significantly different lifetimes and provide an answer to a long-lasting question in the field.
Electro-magnetic weak coupling optical polaron and temperature effect in quantum dot
NASA Astrophysics Data System (ADS)
Tiotsop, M.; Fotue, A. J.; Kenfack, S. C.; Issofa, N.; Wirngo, A. V.; Tabue Djemmo, M. P.; Fotsin, H.; Fai, L. C.
2015-10-01
We investigate the influence of the electric field and magnetic fields on the ground state energy of a polaron in a spherical semiconductor quantum dot (QD) using the modified Lee Low Pines (LLP) method. The numerical results show the increase of the ground state energy with the increase of the electric field and the electron-phonon coupling constant, and the decrease with the magnetic field and the longitudinal confinement length. It is also seen that the temperature is an increasing function of the cyclotron frequency and the coupling constant whereas it decreases with the electric field strength. The modulation of the electric field, the magnetic field and the confinement length leads to the control of decoherence in the system.
NASA Astrophysics Data System (ADS)
Pradhan, S.; Taraphder, A.
2016-10-01
A spinless, extended Falicov-Kimball model in the presence of a perpendicular magnetic field is investigated employing a self-consistent mean-field theory in two dimensions. In the presence of the field the excitonic average Δ =< di † fi > is modified: the exciton responds in subtle different ways for different values of the magnetic flux. We examine the effects of Coulomb interaction and hybridization between the localized and itinerant electrons on the excitonic average, for rational values of the applied magnetic field. The excitonic average is found to get enhanced exponentially with the Coulomb interaction while it saturates at large hybridization. The orbital magnetic field suppresses the excitonic average in general, though a strong commensurability effect of the magnetic flux on the behaviour of the excitonic order parameter is observed.
NASA Astrophysics Data System (ADS)
Li, L. L.; Zarenia, M.; Xu, W.; Dong, H. M.; Peeters, F. M.
2017-01-01
The magnetic-field dependence of the energy spectrum, wave function, binding energy, and oscillator strength of exciton states confined in a circular graphene quantum dot (CGQD) is obtained within the configuration interaction method. We predict that (i) excitonic effects are very significant in the CGQD as a consequence of a combination of geometric confinement, magnetic confinement, and reduced screening; (ii) two types of excitons (intravalley and intervalley) are present in the CGQD because of the valley degree of freedom in graphene; (iii) the intravalley and intervalley exciton states display different magnetic-field dependencies due to the different electron-hole symmetries of the single-particle energy spectra; (iv) with increasing magnetic field, the exciton ground state in the CGQD undergoes an intravalley to intervalley transition accompanied by a change of angular momentum; (v) the exciton binding energy does not increase monotonically with the magnetic field due to the competition between geometric and magnetic confinements; and (vi) the optical transitions of the intervalley and intravalley excitons can be tuned by the magnetic field, and valley-dependent excitonic transitions can be realized in a CGQD.
Energy levels of an anisotropic three-dimensional polaron in a magnetic field
NASA Astrophysics Data System (ADS)
Brancus, D. E.; Stan, G.
2001-06-01
In the context of the improved Wigner-Brillouin theory, the energy levels are found of a Fröhlich polaron in a uniaxial anisotropic polar semiconductor with complex structure, placed in a magnetic field directed either along the optical axis or orthogonal to it. All sources of anisotropy that are contained in the shape of constant-energy surfaces of the bare electron, the electron-optical-phonon interaction, and the frequency spectrum of the extraordinary phonon modes are considered. Analytical results for the electron-phonon interaction correction to the Landau levels below the optical-phonon continuum are given and, numerical results for the magnetic-field dependence of the cyclotron resonance frequency at low temperature are presented for the particular case of the layered semiconductors InSe and GaSe. Although the interaction between the bare electron and quasitransverse optical-phonon modes is weak, these modes play an important role in the pinning of Landau levels. The results given by Das Sarma for a two-dimensional isotropic magnetopolaron are generalized to the anisotropic uniaxial case by taking formally m∥-->∞ in the expression of the perturbed Landau levels found when the magnetic field is directed along the optical axis, m∥ being the component of the bare-electron effective-mass tensor along the optical axis.
Two-Exciton and Exciton-Magnon Bands in DIMANGANESE(+) Magnets.
NASA Astrophysics Data System (ADS)
Darwish, Saqer Mohammed
The temperature dependence of several exciton -magnon and two-exciton bands in the optical absorption spectra of three antiferromagnets have been studied using a Cary 14 spectrophotometer in conjunction with an Air Product Displex, closed-cycle helium refrigerator. The three antiferromagnets with their T_{ rm N} are: KMnF_3, T_{rm N} = 88.3 K; RbMnF_3, T_{ rm N} = 82.6 K; and MnF_2 , T_{rm N} = 67.3 K. In this work the temperature dependence (10 ^circK to 300^ circK) of the line position E, the oscillator strength f, and the half-width of half maximum delta, for several of these bands were measured. For the two-exciton bands f increases where as for the exciton-magnon and exciton-magnon-phonon bands f decreases as the temperature is lowered through T _{rm N}. The temperature dependence of f for the two-exciton bands in the three antiferromagnets agrees well with the theoretical predictions of Fujiwara et al. For the exciton-magnon bands, f increases with increasing T up to T_{rm N} and then remains essentially constant above T_{rm N}, in reasonable agreement with the theory of Shinagawa and Tanabe. For the exciton-magnon-phonon bands, a slight increase in f above T_{rm N} is believed to be due to the role of a phonon. The temperature dependence of the line positions E(T) is also different for the exciton-magnon and two-exciton bands. The exciton-magnon or exciton-magnon-phonon bands undergo a blue shift in E(T) as the temperature is lowered through T_{rm N}. This is semiquantitatively understood in terms of the exchange field using the molecular field theory of Yen et al. On the other hand, most of the two-exciton bands do not show any anomaly in E(T) below T_{rm N}. Instead their line positions are described well by the Einstein-type relation E(T) = E(O) + A ^{*}/ (exp(T^ {*}/T) - 1), where T^{*} represents an odd symmetry phonon with frequency upsilon * = kT^{*} /h. Above T_{rm N} , the exciton-magnon-phonon bands also follow the same equation. From these fits
NASA Astrophysics Data System (ADS)
Barman, Biplob; Oszwaldowski, Rafal; Schweidenback, Lars; Russ, Andreas; Murphy, Joseph; Cartwright, Alexander; Zutic, Igor; McCombe, Bruce; Petrou, Athos; Chou, Wu-Ching; Chung Fan, Wen; Sellers, Ian; Petukhov, Andre
2013-03-01
We have extended our previous investigation of time evolution of PL from (Zn,Mn)Te/ZnSe quantum dots in a magnetic field B. PL studies at T = 5 K in these type-II dots reveal formation of magnetic polarons (MP). We find their formation time τMP to be 0.5 ns, which varies little with B. The circular polarization P of the emission shows a surprising behavior. For all fields, the characteristic time τP is longer than τMP. Furthermore, τP decreases from 10 ns to 1.9 ns as B increases from 1 to 4 tesla. We attribute this effect to a low- B bottleneck in the σ+ recombination channel, due to the almost equal populations of the spin +/- 1 / 2 electrons participating in the interband transitions. In contrast, the +/- 3 / 2 holes in the (Zn,Mn)Te QDs, are affected mostly by the effective field due to exchange interaction between hole and Mn spins around it. This effective field is much larger than B. Work supported by DOE-BES, ONR and NSF.
Ding, Baofu Alameh, Kamal
2014-07-07
The research field of organic spintronics has remarkably and rapidly become a promising research area for delivering a range of high-performance devices, such as magnetic-field sensors, spin valves, and magnetically modulated organic light emitting devices (OLEDs). Plenty of microscopic physical and chemical models based on exciton or charge interactions have been proposed to explain organic magneto-optoelectronic phenomena. However, the simultaneous observation of singlet- and triplet-exciton variations in an external magnetic field is still unfeasible, preventing a thorough theoretical description of the spin dynamics in organic semiconductors. Here, we show that we can simultaneously observe variations of singlet excitons and triplet excitons in an external magnetic field, by designing an OLED structure employing a singlet-exciton filtering and detection layer in conjunction with a separate triplet-exciton detection layer. This OLED structure enables the observation of a Lorentzian and a non-Lorentzian line-shape magnetoresponse for singlet excitons and triplet excitons, respectively.
Exciton condensation in an extended Falicov-Kimball model in the presence of orbital magnetic fields
NASA Astrophysics Data System (ADS)
Pradhan, Subhasree; Taraphder, A.
2016-12-01
We investigate the exciton condensation in the presence of an external, perpendicular magnetic field in a two-dimensional extended spinless Falicov-Kimball model involving itinerant (c) and localized (f) electrons in the half-filled limit, using self-consistent, mean-field approximations. On tuning the orbital magnetic field the excitonic averages Δi =< c_i^\\dagger f_i> are affected in several ways: the external field usually suppresses the excitonic average but we find that it is also possible to enhance excitonic response at some values of the magnetic field. We further examine the effect of Coulomb interaction and the f-electron hopping on the condensation of excitons for some rational values of the applied magnetic fields. The interband Coulomb interaction enhances Δ exponentially and the effect is more pronounced for low hybridization. The strength of excitonic average drops when f-electrons have a dispersion. This trend is independent of the relative sign of the c- and f-electron hopping; although the excitonic response is different for different parity of the c- and f-electrons.
Jahan K, Luhluh Boda, Aalu; Chatterjee, Ashok
2015-05-15
The problem of an exciton trapped in a three dimensional Gaussian quantum dot is studied in the presence of an external magnetic field. A variational method is employed to obtain the ground state energy of the exciton as a function of the quantum dot size, the confinement strength and the magnetic field. It is also shown that the variation of the size of the exciton with the radius of the quantum dot.
A Comparison Between Magnetic Field Effects in Excitonic and Exciplex Organic Light-Emitting Diodes
NASA Astrophysics Data System (ADS)
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.
NASA Astrophysics Data System (ADS)
Berciu, Mona
2014-06-01
We show that even in the presence of a transverse magnetic field, the eigenstates of an exciton remain invariant to the full lattice translation group. This is expected if the exciton is viewed as a neutral quasiparticle, but not if one views it as a bound electron-hole pair. Single electron and hole wave functions are invariant only to the magnetic translation group, and their momenta are restricted to the magnetic Brillouin zone; the associated folding is the origin of their Hofstadter butterfly spectra. We find that such folding is not necessary for exciton eigenstates, which are characterized by momenta in the full Brillouin zone and thus have higher symmetry than the Hamiltonian. The magnetic field can have a significant effect on the shape of the exciton dispersion, however. While similar effects have been noted in continuous models, we find qualitatively different behavior for Frenkel excitons, whose origin we clarify. We also derive an analytical solution for the Hofstadter butterfly on a square lattice and analyze its dispersion in the full Brillouin zone.
NASA Astrophysics Data System (ADS)
Kolodiazhnyi, Taras; Charoonsuk, Thitirat; Seo, Yu-Seong; Chang, Suyong; Vittayakorn, Naratip; Hwang, Jungseek
2017-01-01
We report magnetic susceptibility, electrical conductivity and optical absorption of Ce1 -xMxO2 where M = Nb,Ta and 0 ≤x ≤0.03 . The dc conductivity follows a simple thermally activated Arrhenius-type behavior in the T =70 -700 K range with a change in slope at T*≈155 K. The high-temperature activation energy shows gradual increase from ≈170 to 220 meV as the dopant concentration increases. The activation energy of the low-temperature conductivity shows a broad minimum of ≈77 meV at x ≈0.01 . Electron transport and localization mechanisms are analyzed in the framework of the Holstein small polaron, Anderson localization, and Jahn-Teller distortion models. The fit to the small polaron mobility is dramatically improved when, instead of the longitudinal phonons, the transverse optical phonons are considered in the phonon-assisted electron transport. This serves as an indirect evidence of a strong 4 f1 orbital interaction with the oxygen ligands, similar to the case of PrO2. Based on comparison of the experimental data to the models, it is proposed that the defect-induced random electric fields make the dominant contribution to the electron localization in donor-doped ceria.
NASA Astrophysics Data System (ADS)
Liu, Yun-Fei; Xiao, Jing-Lin
2009-03-01
In a two-dimensional quantum dot (QD) with parabolic confinement potential, we investigate pure dephasing due to deformation potential exciton-bulk longitudinal acoustic phonons (LAP) interaction for exciton qubits under the influence of external static electric and magnetic fields by adopting the full quantum-mechanical method of Kunihiro Kojima and Akihisa Tomita. The wave function is found and the dependence of the pure dephasing factor on the confinement length of the QD and time and temperature is discussed. We find the external electric and magnetic fields have important effects on pure dephasing of exciton qubits because exciton-LAP interaction increases, leading to more pure dephasing.
Quantum vibrational polarons: Crystalline acetanilide revisited
NASA Astrophysics Data System (ADS)
Hamm, Peter; Edler, Julian
2006-03-01
We discuss a refined theoretical description of the peculiar spectroscopy of crystalline acetanilide (ACN). Acetanilide is a molecular crystal with quasi-one-dimensional chains of hydrogen-bonded units, which is often regarded as a model system for the vibrational spectroscopy of proteins. In linear spectroscopy, the CO stretching (amide I) band of ACN features a double-peak structure, the lower of which shows a pronounced temperature dependence which has been discussed in the context of polaron theory. In nonlinear spectroscopy, both of these peaks respond distinctly differently. The lower-frequency band exhibits the anharmonicity expected from polaron theory, while the higher-frequency band responds as if it were quasiharmonic. We have recently related the response of the higher-frequency band to that of a free exciton [J. Edler and P. Hamm, J. Chem. Phys. 117, 2415 (2002)]. However, as discussed in the present paper, the free exciton is not an eigenstate of the full quantum version of the Holstein polaron Hamiltonian, which is commonly used to describe these phenomena. In order to resolve this issue, we present a numerically exact solution of the Holstein polaron Hamiltonian in one dimension (1D) and 3D. In 1D, we find that the commonly used displaced oscillator picture remains qualitatively correct, even for relatively large exciton coupling. However, the result is not in agreement with the experiment, as it fails to explain the free-exciton band. In contrast, when taking into account the 3D nature of crystalline acetanilide, certain parameter regimes exist where the displaced oscillator picture breaks down and states appear in the spectrum that indeed exhibit the characteristics of a free exciton. The appearance of these states is a speciality of vibrational polarons, whose source of exciton coupling is transition dipole coupling which is expected to have opposite signs of interchain and intrachain coupling.
NASA Astrophysics Data System (ADS)
Beaulac, Remi
2010-03-01
An attractive approach to controlling spin effects in semiconductor nanostructures for applications in electronics is to use light to generate, manipulate, or read out spins. The main focus of this presentation will be on the recent demonstration of spontaneous photoinduced polarization of Mn(II) spins in doped colloidal CdSe quantum dots, an effect due to the formation of excitonic magnetic polarons. Photoexcitation generates large dopant-carrier exchange fields, enhanced by strong spatial confinement, that lead to giant Zeeman splittings of the semiconductor band structure in the absence of applied magnetic fields. These internal exchange fields allow spontaneous magnetic saturation of the Mn(II) spins to be achieved at zero external magnetic field up to ca. 50 K, and photomagnetic effects are observed all the way up to room temperature. The factors that allow this fascinating effect to be observed in colloidal Mn(II)-doped CdSe nanoparticles will be discussed. Relevant Publications: 1) Beaulac, Schneider, Archer, Bacher, and Gamelin. Science, 325, 973 (2009) 2) Beaulac, Archer, Ochsenbein, and Gamelin, Adv. Funct. Mat., 18, 3873 (2008)
Abbate, Sergio; Bruhn, Torsten; Pescitelli, Gennaro; Longhi, Giovanna
2017-01-12
The vibrational exciton (VE) interpretation of intense bisignated couplets in vibrational circular dichroism (VCD) spectra of a pair of atropisomeric BODIPY (boron dipyrrin) dimers is discussed. The role of intrinsic magnetic moments is crucial to reproduce the different behaviors of quasi-isomeric BODIPY dimers with different aryl junction.
Sinito, Chiara; Fernée, Mark J; Goupalov, Serguei V; Mulvaney, Paul; Tamarat, Philippe; Lounis, Brahim
2014-11-25
We use nominally spheroidal CdSe nanocrystals with a zinc blende crystal structure to study how shape perturbations lift the energy degeneracies of the band-edge exciton. Nanocrystals with a low degree of symmetry exhibit splitting of both upper and lower bright state degeneracies due to valence band mixing combined with the isotropic exchange interaction, allowing active control of the level splitting with a magnetic field. Asymmetry-induced splitting of the bright states is used to reveal the entire 8-state band-edge fine structure, enabling complete comparison with band-edge exciton models.
Excitonic spin-splitting in quantum wells with a tilted magnetic field.
dos Santos, L Fernandes; Castelano, L K; Padilha, J X; Pusep, Y; Marques, G E; Smirnov, D; Bakarov, A K; Toropov, A I; Lopez-Richard, V
2016-02-10
This work aims to investigate the effects of magnetic field strength and direction on the electronic properties and optical response of GaAs/AlGaAs-based heterostructures. An investigation of the excitonic spin-splitting of a disordered multiple quantum well embedded in a wide parabolic quantum well is presented. The results for polarization-resolved photoluminescence show that the magnetic field dependencies of the excitonic spin-splitting and photoluminescence linewidth are crucially sensitive to magnetic field orientation. Our experimental results are in good agreement with the calculated Zeeman splitting obtained by the Luttinger model, which predicts a hybridization of the spin character of states in the valence band under tilted magnetic fields.
Effective Landé factor in a GaMnAs quantum dot; with the effects of sp-d exchange on a bound polaron
Lalitha, D. Peter, A. John
2014-04-24
The effective g-factor of conduction (valence) band electron (hole) is obtained in the GaMnAs quantum dot. Magneto bound polaron in a GaMnAs/Ga{sub 0.6}Al{sub 0.4}As quantum dot is investigated with the inclusion of exchange interaction effects due to Mn alloy content and the geometrical confinement. The spin polaronic energy of the heavy hole exciton is studied with the spatial confinement using a mean field theory in the presence of magnetic field strength.
Tunable Magnetic Alignment between Trapped Exciton-Polariton Condensates.
Ohadi, H; Del Valle-Inclan Redondo, Y; Dreismann, A; Rubo, Y G; Pinsker, F; Tsintzos, S I; Hatzopoulos, Z; Savvidis, P G; Baumberg, J J
2016-03-11
Tunable spin correlations are found to arise between two neighboring trapped exciton-polariton condensates which spin polarize spontaneously. We observe a crossover from an antiferromagnetic to a ferromagnetic pair state by reducing the coupling barrier in real time using control of the imprinted pattern of pump light. Fast optical switching of both condensates is then achieved by resonantly but weakly triggering only a single condensate. These effects can be explained as the competition between spin bifurcations and spin-preserving Josephson coupling between the two condensates, and open the way to polariton Bose-Hubbard ladders.
A huge renormalization of transport effective mass in the magnetic-polaronic state of EuB 6
NASA Astrophysics Data System (ADS)
Glushkov, V.; Bogach, A.; Demishev, S.; Gon'kov, K.; Ignatov, M.; Khayrullin, Eu.; Samarin, N.; Shubin, A.; Shitsevalova, N.; Flachbart, K.; Sluchanko, N.
2008-04-01
The comprehensive study of galvanomagnetic, thermoelectric and magnetic properties was carried out on the single crystals of low carrier density ferromagnetic metal EuB 6 ( TC≈13.9 K, Tm=15.8 K) in a wide range of temperatures (1.8-300 K) and magnetic fields (up to 80 kOe). The analysis of the microscopic characteristics estimated from the data revealed a giant renormalization of the charge carriers’ effective mass meff, which is observed in the paramagnetic state of this compound with strong electron correlations. The gradual decrease of meff from the maximum of meff∼30 meff detected at T*≈80 K to the low temperature values of meff ( T⩽ TC)∼0.2-1 m0 is discussed in terms of the phase separation with the formation of low resistive ferromagnetic nano-sized regions (ferrons) in the dielectric magnetic polaronic state ( T> Tm). The observed unusual behavior of meff favors recent explanation of the genesis of the metal-insulator transition scenario proposed for La-doped EuB 6 systems [U. Yu, B.I. Min, Phys. Rev. Lett. 94 (2005) 117202.].
Podlesnyak, Andrey A; Ehlers, Georg; Frontzek, Matthias D; Sefat, A. S.; Furrer, Albert; Straessle, Thierry; Pomjakushina, Ekaterina; Conder, Kazimierz; Demmel, F.; Khomskii, D. I.
2011-01-01
We investigate the doping dependence of the nanoscale electronic and magnetic inhomogeneities in the hole-doping range 0.002 < x < 0.1 of cobalt based perovskites, La{sub 1-x}Sr{sub x}CoO{sub 3}. Using single-crystal inelastic neutron scattering and magnetization measurements we show that the lightly doped system exhibits magnetoelectronic phase separation in the form of spin-state polarons. Higher hole doping leads to a decay of spin-state polarons in favor of larger scale magnetic clusters, due to competing ferromagnetic correlations of Co{sup 3+} ions which are formed by neighboring polarons. The present data give evidence for two regimes of magnetoelectronic phase separation in this system: (i) x {approx}< 0.05, dominated by ferromagnetic intrapolaron interactions, and (ii) x {approx}> 0.05, dominated by Co{sup 3+}-Co{sup 3+} intracluster interactions. Our conclusions are in good agreement with a recently proposed model of the phase separation in cobalt perovskites.
Tracking the coherent generation of polaron pairs in conjugated polymers
NASA Astrophysics Data System (ADS)
de Sio, Antonietta; Troiani, Filippo; Maiuri, Margherita; Réhault, Julien; Sommer, Ephraim; Lim, James; Huelga, Susana F.; Plenio, Martin B.; Rozzi, Carlo Andrea; Cerullo, Giulio; Molinari, Elisa; Lienau, Christoph
2016-12-01
The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.
NASA Astrophysics Data System (ADS)
Liu, Guanghui; Guo, Kangxian; Wu, Qingjie; Wu, Jing-He
2013-01-01
Polaron effects on the optical rectification (OR) and the second harmonic generation (SHG) in cylindrical quantum dots (CQDs) with the radial parabolic potential and the z-direction linear potential in the presence of the magnetic field are theoretically investigated. The expressions for both the OR and the SHG are obtained within the framework of the compact-density-matrix approach and the iterative method. After considering the electron-LO-phonon interaction (ELOPI) as perturbation, the energy levels and the wave functions of an electron confined in CQD are obtained by perturbation theory. Numerical calculations are presented for GaAs/AlGaAs. It is found that when we consider the ELOPI, the resonant peak of the OR χ0(2) is enhanced, whereas the magnitude of the SHG χ2ω(2) is greatly enhanced. It is also found that when we ignore the ELOPI, with the increase of the radial confinement frequency ωρ and the magnetic field B, respectively, the resonant peak of the OR χ0(2) remains constant, whereas the magnitude of the SHG χ2ω(2) becomes small. However, when we consider the ELOPI, with the increase of ωρ,B and V respectively, both the resonant peak of the OR χ0(2) and the magnitude of the SHG χ2ω(2) become small. Our results also find that whether the ELOPI is considered or not, with the increase of ωρ, B and V, respectively, both χ0(2) and χ2ω(2) exhibit a blue shift.
NASA Astrophysics Data System (ADS)
Rakshit, Rupali; Serita, Kazunori; Tonouchi, Masayoshi; Mandal, Kalyan
2016-11-01
Herein, terahertz (THz) time domain spectroscopy is used to measure the complex conductivity of semi-insulating CoFe2O4 nanoparticles (NPs) and nano-hollow spheres (NHSs) with different diameters ranging from 100 to 350 nm having a nanocrystalline shell thickness of 19 to 90 nm, respectively. Interestingly, the magnitude of conductivity for CoFe2O4 NPs and NHSs of same average diameter (˜100 nm) for a given frequency of 0.3 THz is found to be 0.33 S/m and 9.08 S/m, respectively, indicating that the hollow structure exhibits greater THz conduction in comparison to its solid counterpart. Moreover, THz conductivity can be tailored by varying the nano-shell thickness of NHSs, and a maximum conductivity of 15.61 S/m is observed at 0.3 THz for NHSs of average diameter 250 nm. A detailed study reveals that thermally activated polaronic hopping plays the key role in determining the electrical transport property of CoFe2O4 nanostructures, which is found to solely depend on their magnitude of THz absorptivity. The non-Drude conductivity of all CoFe2O4 nanostructures is well described by the Polaron model instead of the Drude-Smith model, which is relevant for backscattering of free electrons in a nanostructured material. The Polaron model includes intra-particle and interparticle polaronic conductivities for closely spaced magnetic nanostructures and provides a mean free path of 29 nm for CoFe2O4 NPs of diameter 100 nm, which is comparable with its average crystallite size, indicating the applicability of the developed model for nanomaterials where charge transport is determined by polaronic hopping. Finally, we have demonstrated the morphology and size dependent magnetic measurements of ferrimagnetically aligned CoFe2O4 nanostructures through a vibrating sample magnetometer in the temperature range of 80-250 K, revealing that the disordered surface spin layer of nanostructures significantly controls their magnetism.
Polarons in π-Conjugated Polymers: Anderson or Landau?
Barford, William; Marcus, Max; Tozer, Oliver Robert
2016-02-04
Using both analytical expressions and the density matrix renormalization group method, we study the fully quantized disordered Holstein model to investigate the localization of charges and excitons by vibrational or torsional modes-i.e., the formation of polarons-in conformationally disordered π-conjugated polymers. We identify two distinct mechanisms for polaron formation, namely Anderson localization via disorder (causing the formation of Anderson polarons) and self-localization by self-trapping via normal modes (causing the formation of Landau polarons). We identify the regimes where either description is more valid. The key distinction between Anderson and Landau polarons is that for the latter the particle wave function is a strong function of the normal coordinates, and hence the "vertical" and "relaxed" wave functions are different. This has theoretical and experimental consequences for Landau polarons. Theoretically, it means that the Condon approximation is not valid, and so care needs to be taken when evaluating transition rates. Experimentally, it means that the self-localization of the particle as a consequence of its coupling to the normal coordinates may lead to experimental observables, e.g., ultrafast fluorescence depolarization. We apply these ideas to poly(p-phenylenevinylene). We show that the high frequency C-C bond oscillation only causes Landau polarons for a very narrow parameter regime; generally we expect disorder to dominate and Anderson polarons to be a more applicable description. Similarly, for the low frequency torsional fluctuations we show that Anderson polarons are expected for realistic parameters.
Chang, Wen-Hao; Lin, Chia-Hsien; Fu, Ying-Jhe; Lin, Ta-Chun; Lin, Hsuan; Cheng, Shuen-Jen; Lin, Sheng-Di; Lee, Chien-Ping
2010-01-21
We report on the diamagnetic responses of different exciton complexes in single InAs/GaAs self-assembled quantum dots (QDs) and quantum rings (QRs). For QDs, the imbalanced magnetic responses of inter-particle Coulomb interactions play a crucial role in the diamagnetic shifts of excitons (X), biexcitons (XX), and positive trions (X-). For negative trions (X-) in QDs, anomalous magnetic responses are observed, which cannot be described by the conventional quadratic energy shift with the magnetic field. The anomalous behavior is attributed to the apparent change in the electron wave function extent after photon emission due to the strong Coulomb attraction by the hole in its initial state. In QRs, the diamagnetic responses of X and XX also show different behaviors. Unlike QDs, the diamagnetic shift of XX in QRs is considerably larger than that of X. The inherent structural asymmetry combined with the inter-particle Coulomb interactions makes the wave function distribution of XX very different from that of X in QRs. Our results suggest that the phase coherence of XX in QRs may survive from the wave function localization due to the structural asymmetry or imperfections.
NASA Astrophysics Data System (ADS)
Trojnar, Anna H.; Kadantsev, Eugene S.; Korkusiński, Marek; Hawrylak, Pawel
2011-12-01
A theory of the fine structure of correlated exciton states in self-assembled parabolic semiconductor quantum dots in a magnetic field perpendicular to the quantum dot plane is presented. The correlated exciton wave function is expanded in configurations consisting of products of electron and heavy-hole 2D harmonic oscillator states (HO) in a magnetic field and the electron spin Sz=±1/2 and a heavy-hole spin τz=±3/2 states. Analytical expressions for the short- and long-range electron-hole exchange Coulomb interaction matrix elements are derived in the HO and spin basis for arbitrary magnetic field. This allows the incorporation of short- and long-range electron-hole exchange, direct electron-hole interaction, and quantum dot anisotropy in the exact diagonalization of the exciton Hamiltonian. The fine structure of ground and excited correlated exciton states as a function of a number of confined shells, quantum dot anisotropy, and magnetic field is obtained using exact diagonalization of the many-body Hamiltonian. The effects of correlations are shown to significantly affect the energy splitting of the two bright exciton states.
F Bridges; L Downward; J Neumeier; T Tyson
2011-12-31
We present detailed local structure measurements (using the extended x-ray absorption fine structure technique) for the colossal magnetoresistive material La{sub 1-x}Ca{sub x}MnO{sub 3} (0.21 < x < 0.45) as a function of temperature and magnetic field. The local distortions of the Mn-O bonds are parameterized using {sigma}, the width of the Mn-O pair-distribution function (PDF). After subtracting thermal phonon contributions, we show that the contributions to {sigma}{sup 2} from polaron and Jahn-Teller (JT) distortions, {sigma}{sub JT/polaron}{sup 2}, are a universal function of the magnetization, independent of how the magnetization is achieved via changes in temperature or magnetic field. However this universal behavior is only observed for B fields {ge} 2 T, likely as a result of domain canting in low B fields. The resulting curve is well described by two straight lines with significantly different slopes. These regimes represent two distinctly differ distortions of the oxygen octahedra about the Mn. For low magnetizations up to {approx}65% of the theoretical maximum magnetization, M{sub T}, the slope is low and the distortion removed as the sample becomes magnetized is small - we argue this arises from polarons which have a low distortion around two (or possibly three) Mn sites. At high magnetizations large distortions per Mn site are removed as these sites become magnetized. The data are also analyzed in terms of a two Mn-O peak distribution using experimental standards for Mn-O. The results agree well with recent neutron PDF results but not with some earlier results. We discuss the limitations of assuming a two peak distribution in view of the two distortions needed to describe the Mn-O distortions as a function of T and B for B {ge} 2 T. It is likely that there is a distribution of longer bonds. Finally we show that with increasing B field, the Mn-Mn peak also has a small B-field-induced change - a measure at the unit cell level of magnetostriction but find
High energy sideband on the magnetic polaron related luminescence in EuTe
NASA Astrophysics Data System (ADS)
Heredia, E.; Motisuke, P.; de Oliveira Rappl, P. H.; Brasil, M. J. S. P.; Iikawa, F.
2012-08-01
We investigated the near band gap luminescence of EuTe thin films grown by molecular beam epitaxy, using excitation intensities up to 2 × 105 W/cm2. Besides the previously reported high energy emissions MX1 and MX2, we observed an additional emission band at higher energies. This higher-energy band is only detected when high excitation intensities, over 2 kW/cm2, are used. With increasing externally applied magnetic field, this additional emission band shifts to lower energies at a rate even higher than the MX1. The two bands, however, have different temperature dependences and decay times, suggesting that distinct electronic states are involved in their emission.
NASA Astrophysics Data System (ADS)
Zhu, Liangqing; Shao, Jun; Lin, Tie; Lü, Xiang; Zhu, Junyu; Tang, Xiaodong; Chu, Junhao
2012-04-01
Temperature-dependent magnetic (2-300 K), DC Hall (10-300 K), and infrared transmission (11.5-300 K) measurements are performed on a series of p-type Hg1-xMnxTe (0.12 ≤ x ≤ 0.26) single crystals in the spin-glass regime. Photoionization absorption (PIA) of acceptor-bound magnetic polarons (acceptor-BMPs) is observed to evolve with temperature, which is better accounted for by the classical oscillator model than by the quantum defect method. At low temperatures, p-type Hg1-xMnxTe manifests distinct phenomena of paramagnetic enhancement, negative magnetoresistance, and decrease of the effective binding energy and blueshift of the PIA of the acceptor-BMPs with nearly the same degree as temperature declines. A spin-splitting model is proposed, which can well reproduce the experimentally observed zero-field spin splitting of the acceptor-BMP level at low temperatures and the increase of the spin splitting as temperature drops. The results suggest that the acceptor-BMPs in Hg1-xMnxTe may have potential applications in light-driven polaronic memories, tunable far-infrared lasers, and detectors.
Fermi polaron-polaritons in charge-tunable atomically thin semiconductors
NASA Astrophysics Data System (ADS)
Sidler, Meinrad; Back, Patrick; Cotlet, Ovidiu; Srivastava, Ajit; Fink, Thomas; Kroner, Martin; Demler, Eugene; Imamoglu, Atac
2016-10-01
The dynamics of a mobile quantum impurity in a degenerate Fermi system is a fundamental problem in many-body physics. The interest in this field has been renewed due to recent ground-breaking experiments with ultracold Fermi gases. Optical creation of an exciton or a polariton in a two-dimensional electron system embedded in a microcavity constitutes a new frontier for this field due to an interplay between cavity coupling favouring ultralow-mass polariton formation and exciton-electron interactions leading to polaron or trion formation. Here, we present cavity spectroscopy of gate-tunable monolayer MoSe2 (ref. ) exhibiting strongly bound trion and polaron resonances, as well as non-perturbative coupling to a single microcavity mode. As the electron density is increased, the oscillator strength determined from the polariton splitting is gradually transferred from the higher-energy repulsive exciton-polaron resonance to the lower-energy attractive exciton-polaron state. Simultaneous observation of polariton formation in both attractive and repulsive branches indicates a new regime of polaron physics where the polariton impurity mass can be much smaller than that of the electrons. Our findings shed new light on optical response of semiconductors in the presence of free carriers by identifying the Fermi polaron nature of excitonic resonances and constitute a first step in investigation of a new class of degenerate Bose-Fermi mixtures.
Magnetic-field control of the exciton quantum beats phase in InGaAs/GaAs quantum dots
NASA Astrophysics Data System (ADS)
Siarry, B.; Eble, B.; Bernardot, F.; Grinberg, P.; Testelin, C.; Chamarro, M.; LemaÃ®tre, A.
2015-10-01
We demonstrate here the phase control of the neutral exciton quantum beats in InGaAs/GaAs quantum dots. A longitudinal magnetic field is used as a tuning parameter to change the phase of the oscillations in a deterministic way. This effect arises from the competition between the Zeeman splitting and the electron/hole exchange interaction on the exciton dipole symmetry. To explore this mechanism, we have developed a pump-probe setup based on the optical heterodyne detection of the quantum dots reflectivity allowing one to measure the exciton dynamics from a small quantum dots ensemble (˜300 ). Particular attention is paid to give a detailed theoretical analysis of the measurements. The experimental results are in excellent agreement with the model.
Stier, Andreas V.; Wilson, Nathan P.; Clark, Genevieve; ...
2016-11-09
Excitons in atomically thin semiconductors necessarily lie close to a surface, and therefore their properties are expected to be strongly influenced by the surrounding dielectric environment. However, systematic studies exploring this role are challenging, in part because the most readily accessible exciton parameter—the exciton’s optical transition energy—is largely unaffected by the surrounding medium. Here we show that the role of the dielectric environment is revealed through its systematic influence on the size of the exciton, which can be directly measured via the diamagnetic shift of the exciton transition in high magnetic fields. Using exfoliated WSe2 monolayers affixed to single-mode opticalmore » fibers, we tune the surrounding dielectric environment by encapsulating the flakes with different materials and perform polarized low-temperature magneto-absorption studies to 65 T. The systematic increase of the exciton’s size with dielectric screening, and concurrent reduction in binding energy (also inferred from these measurements), is quantitatively compared with leading theoretical models. Furthermore, these results demonstrate how exciton properties can be tuned in future 2D optoelectronic devices.« less
Stier, Andreas V.; Wilson, Nathan P.; Clark, Genevieve; Xu, Xiaodong; Crooker, Scott A.
2016-11-09
Excitons in atomically thin semiconductors necessarily lie close to a surface, and therefore their properties are expected to be strongly influenced by the surrounding dielectric environment. However, systematic studies exploring this role are challenging, in part because the most readily accessible exciton parameter—the exciton’s optical transition energy—is largely unaffected by the surrounding medium. Here we show that the role of the dielectric environment is revealed through its systematic influence on the size of the exciton, which can be directly measured via the diamagnetic shift of the exciton transition in high magnetic fields. Using exfoliated WSe_{2} monolayers affixed to single-mode optical fibers, we tune the surrounding dielectric environment by encapsulating the flakes with different materials and perform polarized low-temperature magneto-absorption studies to 65 T. The systematic increase of the exciton’s size with dielectric screening, and concurrent reduction in binding energy (also inferred from these measurements), is quantitatively compared with leading theoretical models. Furthermore, these results demonstrate how exciton properties can be tuned in future 2D optoelectronic devices.
NASA Astrophysics Data System (ADS)
Patterson, C. H.
2008-03-01
We report hybrid density functional theory calculations on hole doped Ca2-xNaxCuO2Cl2 performed in 4×4 , 42×42 , and 8×2 supercells with hole concentrations x=0.0625 and x=0.125 . Holes at the lower concentration form small polarons, in which the hole is mainly localized on four oxygen ions surrounding one copper ion. The polaron is a spin one-half ferromagnetic polaron (Cu5O4) , in which the moment on the central copper ion is parallel to those on the four neighboring copper ions and the moment on the oxygen ions is opposed to that on the copper ions. This is therefore an Emery-Reiter spin polaron rather than a Zhang-Rice singlet. At the higher hole concentration (x=0.125) , many cuprates form stripes. Hybrid density functional theory calculations on linear chains of spin polarons separated by 4a0 show a group of bands localized mainly on the stripe. Spins on neighboring copper ions in the stripe are parallel and so the stripe forms a magnetic antiphase boundary between antiferromagnetically ordered blocks of copper spins. Stripes of this kind, which run in one direction only, may explain recent scanning tunneling microscopy data from Ca2-xNaxCuO2Cl2 by Kohsaka [Science 315, 1380 (2007)]. We also consider an ordered spin polaron phase where magnetic antiphase boundaries intersect at right angles. In this case, sets of four copper ions in squares at stripe intersections have parallel spins. This phase may be the 4×4 checkerboard pattern reported by Hanaguri [Nature (London) 430, 1001 (2004)].
NASA Astrophysics Data System (ADS)
Yin, Miao; Cheng, Ze; Wu, Zi-Xia; Ping, Yun-Xia
2009-03-01
Some properties of excitons in polar semiconductors are studied theoretically by means of squeezed state variational approach. This method makes it possible to consider bilinear terms of the phonon operators as well as linear terms arising from the Lee-Low-Pines (LLP)-like transformation. The exciton ground state energy and binding energy are calculated numerically. It is shown that the squeezing effect is significant in the case of strong exciton-phonon coupling region.
Solnyshkov, D. D.; Malpuech, G.; Shelykh, I. A.
2009-10-15
We establish a phase diagram of a spinor exciton-polariton condensate in a disordered microcavity in the presence of an external magnetic field. We find that the combination of the full paramagnetic screening and Anderson localization leads to the formation of a condensed phase having both localized and superfluid components. This is reflected by different dispersions of elementary excitations for the two polarization components.
Semiclassical and quantum polarons in crystalline acetanilide
NASA Astrophysics Data System (ADS)
Hamm, P.; Tsironis, G. P.
2007-08-01
Crystalline acetanilide is a an organic solid with peptide bond structure similar to that of proteins. Two states appear in the amide I spectral region having drastically different properties: one is strongly temperature dependent and disappears at high temperatures while the other is stable at all temperatures. Experimental and theoretical work over the past twenty five years has assigned the former to a selftrapped state while the latter to an extended free exciton state. In this article we review the experimental and theoretical developments on acetanilide paying particular attention to issues that are still pending. Although the interpretation of the states is experimentally sound, we find that specific theoretical comprehension is still lacking. Among the issues that that appear not well understood is the effective dimensionality of the selftrapped polaron and free exciton states.
NASA Astrophysics Data System (ADS)
Scott, Alwyn C.; Bigio, Irving J.; Johnston, Clifford T.
1989-06-01
The best available data are presented of the integrated intensity of the 1650-cm-1 band in crystalline acetanilide as a function of temperature. A concise theory of polaron states is presented and used to interpret the data.
Scott, A. C.; Bigio, I. J.; Johnston, C. T.
1989-06-15
The best available data are presented of the integrated intensity of the1650-cm/sup /minus/1/ band in crystalline acetanilide as a function oftemperature. A concise theory of polaron states is presented and used tointerpret the data.
Magnon Polarons in the Spin Seebeck Effect.
Kikkawa, Takashi; Shen, Ka; Flebus, Benedetta; Duine, Rembert A; Uchida, Ken-Ichi; Qiu, Zhiyong; Bauer, Gerrit E W; Saitoh, Eiji
2016-11-11
Sharp structures in the magnetic field-dependent spin Seebeck effect (SSE) voltages of Pt/Y_{3}Fe_{5}O_{12} at low temperatures are attributed to the magnon-phonon interaction. Experimental results are well reproduced by a Boltzmann theory that includes magnetoelastic coupling. The SSE anomalies coincide with magnetic fields tuned to the threshold of magnon-polaron formation. The effect gives insight into the relative quality of the lattice and magnetization dynamics.
Magnon Polarons in the Spin Seebeck Effect
NASA Astrophysics Data System (ADS)
Kikkawa, Takashi; Shen, Ka; Flebus, Benedetta; Duine, Rembert A.; Uchida, Ken-ichi; Qiu, Zhiyong; Bauer, Gerrit E. W.; Saitoh, Eiji
2016-11-01
Sharp structures in the magnetic field-dependent spin Seebeck effect (SSE) voltages of Pt /Y3Fe5 O12 at low temperatures are attributed to the magnon-phonon interaction. Experimental results are well reproduced by a Boltzmann theory that includes magnetoelastic coupling. The SSE anomalies coincide with magnetic fields tuned to the threshold of magnon-polaron formation. The effect gives insight into the relative quality of the lattice and magnetization dynamics.
NASA Astrophysics Data System (ADS)
Singh, Sunny; Kaur, Harsimran; Sharma, Shivalika; Aggarwal, Priyanka; Hazra, Ram Kuntal
2017-04-01
The understanding of the physics of exciton, bi-exciton, tri-exciton and the subsequent insight into controlling the properties of mesoscopic systems holds the key to various exotic optical, electrical and magnetic phenomena like superconductivity, Mott insulation, Quantum Hall effect etc. Many of exciton properties are similar to atomic hydrogen that attracts researchers to explore electronic structure of exciton in quantum dots, but nontriviality arises due to coulombic interactions among electrons and holes. We propose an exact integral of coulomb (exchange) correlation in terms of finitely summed Lauricella functions to examine 3-D exciton of harmonic dots confined in zero and non-zero arbitrary magnetic field. The highlight of our work is the use of exact variational solution for coloumbic interaction between the hole and the electron and evaluation of the cross terms arising out of the coupling among centre-of-mass and relative coordinates. We also have extended the size of the system to generalized N-body problem with N=3,4 for tri-exciton (e-e-h/e-h-h)
Verma, Kuldeep Chand; Kotnala, R K
2016-02-21
Zn0.94TM0.03Ce0.03O [Zn0.94Fe0.03Ce0.03O (ZFCeO) and Zn0.94Co0.03Ce0.03O (ZCCeO)] nanoparticles were synthesized by a sol-gel process. Elemental analysis of these nanoparticles detects the weight percentage of Zn, Co, Fe, Ce and O in each sample. The Rietveld refinement of the X-ray diffraction pattern obtains the occupancy of dopant atoms, Wurtzite ZnO structure, crystallinity and lattice deformation with doping. The Ce doping into ZFO and ZCO form nanoparticles than nanorods was observed in pure ZnO, ZFO and ZCO samples that described due to chemical and ionic behavior of Ce, Fe, Co and Zn ions. The Raman active modes have peak broadening, intensity changes and peak shifts with metal doping that induces lattice defects. Photoluminescence spectra show blue-shifts at near-band edges and defects that influence broad visible emission with Ce doping. An enhancement in ferromagnetism in the magnetic hysteresis at 5 K is measured. The zero-field cooling and field cooling at H = 500 Oe and T = 300-5 K could confirm antiferromagnetic interactions mediated by defect carriers. The bound magnetic polaron at defect sites is responsible for the observed ferromagnetism. The ac magnetic susceptibility measurements determine the antiferromagnetic to ferromagnetic transition with some magnetic clustered growth in the samples and reveal a frequency independent peak that shows the Neel temperature. Weak room temperature ferromagnetism and optical quenching in ZFCeO are described by valance states of Fe and Ce ions, respectively. Using first-principle calculations, we studied the occupancy of Ce (replacing Zn atoms) in the Wurtzite structure.
Tracking the coherent generation of polaron pairs in conjugated polymers
De Sio, Antonietta; Troiani, Filippo; Maiuri, Margherita; Réhault, Julien; Sommer, Ephraim; Lim, James; Huelga, Susana F.; Plenio, Martin B.; Rozzi, Carlo Andrea; Cerullo, Giulio; Molinari, Elisa; Lienau, Christoph
2016-01-01
The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials. PMID:27929115
Tracking the coherent generation of polaron pairs in conjugated polymers.
De Sio, Antonietta; Troiani, Filippo; Maiuri, Margherita; Réhault, Julien; Sommer, Ephraim; Lim, James; Huelga, Susana F; Plenio, Martin B; Rozzi, Carlo Andrea; Cerullo, Giulio; Molinari, Elisa; Lienau, Christoph
2016-12-08
The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.
Hoang-Do, Ngoc-Tram; Hoang, Van-Hung; Le, Van-Hoang
2013-05-15
The Feranchuk-Komarov operator method is developed by combining with the Levi-Civita transformation in order to construct analytical solutions of the Schroedinger equation for a two-dimensional exciton in a uniform magnetic field of arbitrary strength. As a result, analytical expressions for the energy of the ground and excited states are obtained with a very high precision of up to four decimal places. Especially, the precision is uniformly stable for the whole range of the magnetic field. This advantage appears due to the consideration of the asymptotic behaviour of the wave-functions in strong magnetic field. The results could be used for various physical analyses and the method used here could also be applied to other atomic systems.
Pulsed magnetic field study of the spin gap in intermediate valence compound SmB 6
NASA Astrophysics Data System (ADS)
Flachbart, K.; Bartkowiak, M.; Demishev, S.; Gabani, S.; Glushkov, V.; Herrmannsdorfer, T.; Moshchalkov, V.; Shitsevalova, N.; Sluchanko, N.
2009-10-01
In this work, we report the behavior of electrical resistivity of SmB 6 at temperatures between 2.2 and 70 K in pulsed magnetic fields up to 54 T. A strong negative magnetoresistance was detected with increasing magnetic field, when lowering the temperature in the range T<30 K. We show that the amplitude of negative magnetoresistance reaches its maximum dR/R~70% at B=54 T, in the vicinity of phase transition occurring in this strongly correlated electron system at TC~5 K. The crossover from negative magnetoresistance to positive magnetoresistance found at intermediate temperatures at T>30 K is discussed within the framework of exciton-polaron model of local charge fluctuations in SmB 6 proposed by Kikoin and Mishchenko. It seems that these exciton-polaron in-gap states are influenced both by temperature and magnetic field.
Excitons in coupled type-II double quantum wells under electric and magnetic fields: InAs/AlSb/GaSb
Lyo, S. K.; Pan, W.
2015-11-21
We calculate the wave functions and the energy levels of an exciton in double quantum wells under electric (F) and magnetic (B) fields along the growth axis. The result is employed to study the energy levels, the binding energy, and the boundary on the F–B plane of the phase between the indirect exciton ground state and the semiconductor ground state for several typical structures of the type-II quasi-two-dimensional quantum wells such as InAs/AlSb/GaSb. The inter-well inter-band radiative transition rates are calculated for exciton creation and recombination. We find that the rates are modulated over several orders of magnitude by the electric and magnetic fields.
Mrowiński, P.; Musiał, A.; Maryński, A.; Syperek, M.; Misiewicz, J.; Sęk, G.; Somers, A.; Reithmaier, J. P.; Höfling, S.
2015-02-02
We investigated the neutral and charged exciton fine structure in single InAs/InGaAlAs/InP quantum dashes emitting at 1.55 μm using polarization-resolved microphotoluminescence in a magnetic field. Inverted spin configuration of horizontally [1–10] and vertically [110] polarized transitions has been observed. An in-plane magnetic field of up to 5 Tesla has been applied to tailor the fine structure, and eventually to reduce the splitting of the bright exciton states down to zero. This inverted structure has been observed for all the investigated excitons, making it a characteristic feature for this class of nanostructures with the largest splitting reduction of 170 μeV.
Snedden, Edward W; Monkman, Andrew P; Dias, Fernando B
2013-04-04
Geminate polaron-pair recombination directly to the triplet state of the small dye molecule copper(II) 1,4,8,11,15,18,22,25-octabutoxy-29H,31H- phthalocyanine (CuPC) and exciton trapping in CuPC domains, combine to reduce the internal quantum efficiency of free polaron formation in the bulk-heterojunction blends of CuPC doped with [6,6]-phenyl-C61-butyric acid methyl ester (PCBM) as the electron acceptor.
Ultrafast generation of pseudo-magnetic field for valley excitons in WSe2 monolayers
NASA Astrophysics Data System (ADS)
Kim, Jonghwan; Hong, Xiaoping; Jin, Chenhao; Shi, Su-Fei; Chang, Chih-Yuan S.; Chiu, Ming-Hui; Li, Lain-Jong; Wang, Feng
2015-03-01
The valley pseudospin emerges as a new degree of freedom in atomically thin two-dimensional transition metal dichalcogenides (MX2). In analogy to the control of spin in spintronics, the capability to manipulate the valley pseudospin can provide exciting opportunities in valleytronics. Here we present that femtosecond pulses with circular polarization can generate ultrafast and ultrahigh valley pseudomagnetic field in a monolayer MX2. Our polarization-resolved transient absorption measurement shows that the degeneracy of valley exciton transitions at K and K' valley in WSe2 monolayers can be lifted by optical Stark effect from the non-resonant pump. Energy splitting due to the optical Stark effect is linear with both the pump intensity and the inverse of pump detuning. We observe that valley-selective optical Stark effect can create an energy splitting more than 10 meV which corresponds to a pseudomagnetic field over 60 Tesla. Our study demonstrates efficient and ultrafast control of the valley excitons with optical light which can open up the possibility of coherent manipulation of the valley polarization in MX2.
Polaron stability in oligoacene crystals.
Pereira Junior, Marcelo Lopes; Ribeiro Junior, Luiz Antonio
2017-03-01
The polaron stability in organic molecular crystals is theoretically investigated in the scope of a two-dimensional Holstein-Peierls model that includes lattice relaxation. Particularly, the investigation is focused on designing a model Hamiltonian that can address properly the polaron properties in different model oligoacene crystals. The findings showed that a suitable choice for a set of parameters can play the role of distinguishing the model crystals and, consequently, different properties related to the polaron stability in these systems are observed. Importantly, the usefulness of this model is stressed by investigating the electronic localization of the polaron, which provides a deeper understanding into the properties associated with the polaron stability in oligoacene crystals.
NASA Astrophysics Data System (ADS)
Xu, Dazhi; Cao, Jianshu
2016-08-01
The concept of polaron, emerged from condense matter physics, describes the dynamical interaction of moving particle with its surrounding bosonic modes. This concept has been developed into a useful method to treat open quantum systems with a complete range of system-bath coupling strength. Especially, the polaron transformation approach shows its validity in the intermediate coupling regime, in which the Redfield equation or Fermi's golden rule will fail. In the polaron frame, the equilibrium distribution carried out by perturbative expansion presents a deviation from the canonical distribution, which is beyond the usual weak coupling assumption in thermodynamics. A polaron transformed Redfield equation (PTRE) not only reproduces the dissipative quantum dynamics but also provides an accurate and efficient way to calculate the non-equilibrium steady states. Applications of the PTRE approach to problems such as exciton diffusion, heat transport and light-harvesting energy transfer are presented.
Magnetic Field Induced Charged Exciton Studies in a GaAs/Al(0.3)Ga(0.7)As Single Heterojunction
Kim, Yongmin; Munteanu, F.M.; Perry, C.H.; Reno, J.L.; Rickel, D.G.; Simmons, J.A.
1999-05-25
The magnetophotoluminescence (MPL) behavior of a GaAs/Al_{0.3}Ga_{0.7}As single heterojunction has been investigated to 60T. We observed negatively charged singlet and triplet exciton states that are formed at high magnetic fields beyond the {nu}=l quantum Hall state. The variation of the charged exciton binding energies are in good agreement with theoretical predictions. The MPL transition intensities for these states showed intensity variations (maxima and minima) at the {nu}=l/3 and 1/5 fractional quantum Hall (FQH) state as a consequence of a large reduction of electron-hole screening at these filling factors.
TOPICAL REVIEW: O- bound small polarons in oxide materials
NASA Astrophysics Data System (ADS)
Schirmer, O. F.
2006-11-01
Holes bound to acceptor defects in oxide crystals are often localized by lattice distortion at just one of the equivalent oxygen ligands of the defect. Such holes thus form small polarons in symmetric clusters of a few oxygen ions. An overview on mainly the optical manifestations of those clusters is given. The article is essentially divided into two parts: the first one covers the basic features of the phenomena and their explanations, exemplified by several paradigmatic defects; in the second part numerous oxide materials are presented which exhibit bound small polaron optical properties. The first part starts with summaries on the production of bound hole polarons and the identification of their structure. It is demonstrated why they show strong, wide absorption bands, usually visible, based on polaron stabilization energies of typically 1 eV. The basic absorption process is detailed with a fictitious two-well system. Clusters with four, six and twelve equivalent ions are realized in various oxide compounds. In these cases several degenerate optically excited polaron states occur, leading to characteristic final state resonance splittings. The peak energies of the absorption bands as well as the sign of the transfer energy depend on the topology of the clusters. A special section is devoted to the distinction between interpolaron and intrapolaron optical transitions. The latter are usually comparatively weak. The oxide compounds exhibiting bound hole small polaron absorptions include the alkaline earth oxides (e.g. MgO), BeO and ZnO, the perovskites BaTiO3 and KTaO3, quartz, the sillenites (e.g. Bi12TiO20), Al2O3, LiNbO3, topaz and various other materials. There are indications that the magnetic crystals NiO, doped with Li, and LaMnO3, doped with Sr, also show optical features caused by bound hole polarons. Beyond being elementary paradigms for the properties of small polarons in general, the defect species treated can be used to explain radiation and light
Chain Length Dependence of Energies of Electron and Triplet Polarons in Oligofluorenes
Chen, Hung Cheng; Sreearunothai, Paiboon; Cook, Andrew R.; ...
2017-03-01
Bimolecular equilibria measured the one-electron reduction potentials and triplet free energies (ΔG°T) of oligo(9,9-dihexyl)fluorenes and a polymer with lengths of n = 1–10 and 57 repeat units. We can accurately measure one-electron potentials electrochemically only for the shorter oligomers. Starting at n = 1 the free energies change rapidly with increasing length and become constant for lengths longer than the delocalization length. Both the reduction potentials and triplet energies can be understood as the sum of a free energy for a fixed polaron and a positional entropy. Furthermore, the positional entropy increases gradually with length beyond the delocalization length duemore » to the possible occupation sites of the charge or the triplet exciton. Our results reinforce the view that charges and triplet excitons in conjugated chains exist as polarons and find that positional entropy can replace a popular empirical model of the energetics.« less
NASA Astrophysics Data System (ADS)
Jeon, H. C.; Kang, T. W.; Kim, T. W.; Cho, Y. H.
2006-06-01
(Ga 1- xMn x)N thin films grown on GaN buffer layers by using molecular beam epitaxy were investigated with the goal of producing diluted magnetic semiconductors (DMSs) with band-edge exciton transitions for applications in optomagnetic devices. The magnetization curve as a function of the magnetic field at 5 K indicated that ferromagnetism existed in the (Ga 1- xMn x)N thin films, and the magnetization curve as a function of the temperature showed that the ferromagnetic transition temperature of the (Ga 1- xMn x)N thin film was above room temperature. Photoluminescence and photoluminescence excitation spectra showed that band-edge exciton transitions in (Ga 1- xMn x)N thin films appeared. These results indicate that the (Ga 1- xMn x)N DMSs with a magnetic single phase hold promise for potential applications in spin optoelectronic devices in the blue region of the spectrum.
NASA Astrophysics Data System (ADS)
Chacham, Helio; Alexandre, Simone S.; Soler, Jose M.; Artacho, Emilio
2004-03-01
The phenomenon of charge transport in DNA has been attracting attention of both biologists and physicists. From the biology side, there are evidences that charge injection can be associated to damage, mutation, and repair processes in DNA. From the physical sciences side, recent developments in nanotechnology now allow the measurement of currents through single DNA molecules in dried samples, which depict semiconductor behavior. Several mechanisms have been proposed for charge migration and transport in DNA. In that respect, detailed electrical transport measurements through DNA molecules containing identical base pairs (poly(dA)-poly(dT) and poly(dG)-poly(dC)) have been recently reported by Yoo et al [1]. These results fit extremely well a model in which the conduction is due to small polaron motion. In particular, these results indicate that the I-V characteristic of poly(dG)-poly(dC) DNA above 200 K is consistent with a small polaron hopping regime with an activation energy of 0.12 eV. In this work [2] we investigate the polaron formation in dry DNA by applying ab initio calculations to both neutral and charged fragments of dry poly(dG)-poly(dC). Our calculations show that the hole polaron in dry poly(dG)-poly(dC) DNA is a clear case of small polaron. This is verified by four basic properties: (i) the small variation of the polaron binding energy as a function of the DNA fragment size, for small fragment sizes, which is an indication of polaron localization; (ii) the fact that the width of the uppermost valence band is an order of magnitude smaller than the polaron binding energy; (iii) the explicit localization of the hole wavefunction for the largest considered fragment (four base pairs), indicated by the fact that about half of the norm of the hole is localized on a single guanine site; (iv) the localization of structural deformations at the nucleotides where the hole is concentrated. Our calculations also give a polaron binding energy of 0.30 eV. This allows
Some approaches to polaron theory
NASA Astrophysics Data System (ADS)
Bogolubov, N. N.; Bogolubov, N. N.
1985-11-01
Here, in our approximation of polaron theory, we examine the importance of introducing the T product, which turn out to be a very convenient theoretical approach for the calculation of thermodynamical averages. We focus attention on the investigation of the so-called linear polaron Hamiltonian and present in detail the calculation of the correlation function, spectral function, and Green function for such a linear system. It is shown that the linear polaron Hamiltonian provides an exactly solvable model of our system, and the result obtained with this approach holds true for an arbitrary coupling constant which describes the strength of interaction between the electron and the lattice vibrations. Then, with the help of a variational technique, we show the possibility of reducing the real polaron Hamiltonian to a socalled trial or approximate linear model Hamiltonian. We also consider the exact calculation of free energy with a special technique that reduces calculations with the help of the T product, which, in our opinion, works much better and is easier than other analogous considerations, for example, the path-integral or Feynman-integral method.(1,2) Here we furthermore recall our own work,(4) where it was shown that the results of Refs. 7 and 8 concerning the impedance calculation in the polaron model may be obtained directly without the use of the path-integral method. The study of the polaron system's thermodynamics is carried out by us in the framework of the functional method. A calculation of the free energy and the momentum distribution function is proposed. Note also that the polaron systems with strong coupling(9) proved to be useful in different quantum field models in connection with the construction of dynamical models of composite particles. A rigorous solution of the special strong-coupling polaron problem, describing the interaction of a nonrelativistic particle with a quantum field, was given by Bogolubov.(3) The works of Tavkhelidze, Fedyanin
Resonant magnetic exciton mode in the heavy-fermion antiferromagnet CeB₆.
Friemel, G; Li, Yuan; Dukhnenko, A V; Shitsevalova, N Y; Sluchanko, N E; Ivanov, A; Filipov, V B; Keimer, B; Inosov, D S
2012-05-15
Resonant magnetic excitations are recognised as hallmarks of unconventional superconductivity in copper oxides, iron pnictides and heavy-fermion compounds. Model calculations have related these modes to the microscopic properties of the pair wave function, but the mechanisms of their formation are still debated. Here we report the discovery of a similar resonant mode in the non-superconducting antiferromagnetic heavy-fermion metal CeB(6). Unlike conventional magnons, the mode is non-dispersive and is sharply peaked around a wave vector separate from those characterising the antiferromagnetic order. It is likely associated with a co-existing order parameter of the unusual antiferro-quadrupolar phase of CeB(6), which has long remained hidden to neutron-scattering probes. The mode energy increases continuously below the onset temperature for antiferromagnetism, in parallel to the opening of a nearly isotropic spin gap throughout the Brillouin zone. These attributes are similar to those of the resonant modes in unconventional superconductors. This unexpected commonality between the two disparate ground states indicates the dominance of itinerant spin dynamics in the ordered low-temperature phases of CeB(6) and throws new light on the interplay between antiferromagnetism, superconductivity and 'hidden' order parameters in correlated-electron materials.
Walker, P; Liew, T C H; Sarkar, D; Durska, M; Love, A P D; Skolnick, M S; Roberts, J S; Shelykh, I A; Kavokin, A V; Krizhanovskii, D N
2011-06-24
A key property of equilibrium exciton-polariton condensates in semiconductor microcavities is the suppression of the Zeeman splitting under a magnetic field. By studying magnetophotoluminescence spectra from a GaAs microcavity, we show experimentally that a similar effect occurs in a nonequilibrium polariton condensate arising from polariton parametric scattering. In this case, the quenching of Zeeman splitting is related to a phase synchronization of spin-up and spin-down polarized polariton condensates caused by a nonlinear coupling via the coherent pump state.
Polaron in a Quasi 0D Nanocrystal
NASA Astrophysics Data System (ADS)
Fai, L. C.; Fotue, A. J.; Mborong, V. B.; Domngang, S.; Issofa, N.; Tchassem, D.
2005-01-01
Polaron states in a spherical quantum dot with a spherical symmetric parabolic confinement potential are investigated applying the Feynman variational principle. Effects of the dot radius on the polaron ground state energy level, the self-action potential energy, the mass and the Fröhlich electron phonon-coupling constant are obtained for a spherical quantum dot. The electron phonon-coupling amplitude derived from the Maxwell equation in a material medium is used. This yields a better upper bound for strong coupling polaron energy in a spherical quantum dot. The polaron mass, energy and self-action potential energy are found to have a monotonous decrease as the structures' radius increases. As the spherical quantum dot radius is reduced the regimes of weak and intermediate coupling polaron shorten and the strong coupling polaron region broadens and extends into weak and intermediate ones. The main contribution to polaron energy and mass comes from the self-action potential.
NASA Astrophysics Data System (ADS)
Gao, Bin; Weng, Yakui; Zhang, Jun-Jie; Zhang, Huimin; Zhang, Yang; Dong, Shuai
2017-03-01
Oxides with 4d/5d transition metal ions are physically interesting for their particular crystalline structures as well as the spin–orbit coupled electronic structures. Recent experiments revealed a series of 4d/5d transition metal oxides R 3 MO7 (R: rare earth; M: 4d/5d transition metal) with unique quasi-one-dimensional M chains. Here first-principles calculations have been performed to study the electronic structures of La3OsO7 and La3RuO7. Our study confirm both of them to be Mott insulating antiferromagnets with identical magnetic order. The reduced magnetic moments, which are much smaller than the expected value for ideal high-spin state (3 t 2g orbitals occupied), are attributed to the strong p ‑ d hybridization with oxygen ions, instead of the spin–orbit coupling. The Ca-doping to La3OsO7 and La3RuO7 can not only modulate the nominal carrier density but also affect the orbital order as well as the local distortions. The Coulombic attraction and particular orbital order would prefer to form polarons, which might explain the puzzling insulating behavior of doped 5d transition metal oxides. In addition, our calculations predict that the Ca-doping can trigger ferromagnetism in La3RuO7 but not in La3OsO7.
Spin dynamics of polarons and polaron pairs in a random hyperfine field
NASA Astrophysics Data System (ADS)
Roundy, Robert C.
Spin-dependent recombination of polaron pairs and spin relaxation of a single polaron are the most fundamental processes are responsible for the performance of organic spintronics-based devices such as light-emitting diodes and organic spin valves. In organic materials, with no spin-orbit coupling, both processes are due to random hyperfine fields created by protons neighboring the polaron sites. The essence of spin-dependent recombination is that in order to recombine the pair must be in the singlet state. Hyperfine fields acting on the electron and hole govern the spin-dynamics of localized pairs during the waiting time for recombination. We demonstrate that for certain domain of trapping configurations of hyperfine fields, crossover to the singlet state is quenched. This leads to the blocking of current. The phenomenon of organic magnetoresistance (OMAR) is described by counting the weights of trapping configurations as a function of magnetic field. This explains the universality of the lineshapes of the OMAR curves. In finite samples incomplete averaging over the hyperfine fields gives rise to mesoscopic fluctuations of the current response. We also demonstrate that under the condition of magnetic resonance, new trapping configurations emerge. This leads to nontrivial evolution of current through the sample with microwave power. When discussing spin-relaxation two questions can be asked: (a) How does the local spin polarization decay as a function of distance from the spin-polarized injector? (b) How does the injected spin decay as a function of time after spatial averaging? With regard to (a), we demonstrate that, while decaying exponentially on average, local spin-polarization exhibits giant fluctuations from point to point. Concerning (b), we find that for a spin-carrier which moves diffusively in low dimensions the decay is faster than a simple exponent. The underlying physics for both findings is that in describing spin evolution it is necessary to add up
Singlet exciton fission photovoltaics.
Lee, Jiye; Jadhav, Priya; Reusswig, Philip D; Yost, Shane R; Thompson, Nicholas J; Congreve, Daniel N; Hontz, Eric; Van Voorhis, Troy; Baldo, Marc A
2013-06-18
Singlet exciton fission, a process that generates two excitons from a single photon, is perhaps the most efficient of the various multiexciton-generation processes studied to date, offering the potential to increase the efficiency of solar devices. But its unique characteristic, splitting a photogenerated singlet exciton into two dark triplet states, means that the empty absorption region between the singlet and triplet excitons must be filled by adding another material that captures low-energy photons. This has required the development of specialized device architectures. In this Account, we review work to develop devices that harness the theoretical benefits of singlet exciton fission. First, we discuss singlet fission in the archetypal material, pentacene. Pentacene-based photovoltaic devices typically show high external and internal quantum efficiencies. They have enabled researchers to characterize fission, including yield and the impact of competing loss processes, within functional devices. We review in situ probes of singlet fission that modulate the photocurrent using a magnetic field. We also summarize studies of the dissociation of triplet excitons into charge at the pentacene-buckyball (C60) donor-acceptor interface. Multiple independent measurements confirm that pentacene triplet excitons can dissociate at the C60 interface despite their relatively low energy. Because triplet excitons produced by singlet fission each have no more than half the energy of the original photoexcitation, they limit the potential open circuit voltage within a solar cell. Thus, if singlet fission is to increase the overall efficiency of a solar cell and not just double the photocurrent at the cost of halving the voltage, it is necessary to also harvest photons in the absorption gap between the singlet and triplet energies of the singlet fission material. We review two device architectures that attempt this using long-wavelength materials: a three-layer structure that uses
Microscopic theories of excitons and their dynamics
NASA Astrophysics Data System (ADS)
Berkelbach, Timothy C.
those that evolve "fast" and "slow," as compared to the internal system dynamics. This method is tested and applied to the spin-boson model, a two-site Frenkel exciton model, and the seven-site Fenna-Matthews-Olson complex. I conclude with a collaborative analysis of a recently developed polaron-transformed quantum master equation, which is shown to accurately interpolate between the well-known Redfield and Forster theories, even in challenging donor-bridge-acceptor arrangements.
Dow, J. D.; Hjalmarson, H. P.; Sankey, O. F.; Allen, R. E.; Buettner, H.
1980-01-01
The observation of core excitons with binding energies much larger than those of the valence excitons in the same material has posed a long-standing theoretical problem. A proposed solution to this problem is presented, and Frenkel excitons and Wannier excitons are shown to coexist naturally in a single material. (GHT)
Ballistic spin transport in exciton gases
NASA Astrophysics Data System (ADS)
Kavokin, A. V.; Vladimirova, M.; Jouault, B.; Liew, T. C. H.; Leonard, J. R.; Butov, L. V.
2013-11-01
Traditional spintronics relies on spin transport by charge carriers, such as electrons in semiconductor crystals. The challenges for the realization of long-range electron spin transport include rapid spin relaxation due to electron scattering. Scattering and, in turn, spin relaxation can be effectively suppressed in excitonic devices where the spin currents are carried by electrically neutral bosonic quasiparticles: excitons or exciton-polaritons. They can form coherent quantum liquids that carry spins over macroscopic distances. The price to pay is a finite lifetime of the bosonic spin carriers. We present the theory of exciton ballistic spin transport which may be applied to a range of systems supporting bosonic spin transport, in particular to indirect excitons in coupled quantum wells. We describe the effect of spin-orbit interaction for the electron and the hole on the exciton spin, account for the Zeeman effect induced by external magnetic fields and long-range and short-range exchange splittings of the exciton resonances. We also consider exciton transport in the nonlinear regime and discuss the definitions of the exciton spin current, polarization current, and spin conductivity.
Band Structures of Plasmonic Polarons
NASA Astrophysics Data System (ADS)
Caruso, Fabio; Lambert, Henry; Giustino, Feliciano
2015-03-01
In angle-resolved photoemission spectroscopy (ARPES), the acceleration of a photo-electron upon photon absorption may trigger shake-up excitations in the sample, leading to the emission of phonons, electron-hole pairs, and plasmons, the latter being collective charge-density fluctuations. Using state-of-the-art many-body calculations based on the `GW plus cumulant' approach, we show that electron-plasmon interactions induce plasmonic polaron bands in group IV transition metal dichalcogenide monolayers (MoS2, MoSe2, WS2, WSe2). We find that the energy vs. momentum dispersion relations of these plasmonic structures closely follow the standard valence bands, although they appear broadened and blueshifted by the plasmon energy. Based on our results we identify general criteria for observing plasmonic polaron bands in the angle-resolved photoelectron spectra of solids.
Polaron assisted charge transfer in model biological systems
NASA Astrophysics Data System (ADS)
Li, Guangqi; Movaghar, Bijan
2016-11-01
We use a tight binding Hamiltonian to simulate the electron transfer from an initial charge-separating exciton to a final target state through a two-arm transfer model. The structure is copied from the model frequently used to describe electron harvesting in photosynthesis (photosystems I). We use this network to provide proof of principle for dynamics, in quantum system/bath networks, especially those involving interference pathways, and use these results to make predictions on artificially realizable systems. Each site is coupled to the phonon bath via several electron-phonon couplings. The assumed large energy gaps and weak tunneling integrals linking the last 3 sites give rise to"Stark Wannier like" quantum localization; electron transfer to the target cluster becomes impossible without bath coupling. As a result of the electron-phonon coupling, local electronic energies relax when the site is occupied, and transient polaronic states are formed as photo-generated electrons traverse the system. For a symmetric constructively interfering two pathway network, the population is shared equally between two sets of equivalent sites and therefore the polaron energy shift is smaller. The smaller energy shift however makes the tunnel transfer to the last site slower or blocks it altogether. Slight disorder (or thermal noise) can break the symmetry, permitting essentially a "one path", and correspondingly more efficient transfer.
Magnetic Field Induced Type-II σ- Excitons in ZnSe/Zn_1-x-yCd_xMn_ySe Quantum Well Structures.
NASA Astrophysics Data System (ADS)
Yu, W. Y.; Salib, M. S.; Petrou, A.; Jonker, B. T.; Warnock, J.
1996-03-01
A magneto-optical study (reflectance and Photoluminescence) of two MBE-grown (100ÅÅZnSe/Zn_1-x-yCd_xMn_ySe Quantum Well Structures has been carried out. Both samples are Type-I at zero magnetic field with electrons and holes confined in the ZnCdMnSe layers^1. In the x=0.03, y=0.04 structure, the magnetic field induced valence band splittings confine the m_j=+3/2(-3/2) hole in the ZnSe(ZnCdMnSe) layers; both electron spin states (m_j=±1/2) are confined in the ZnCdMnSe layers. For B>3 tesla, the σ- (+1/2, +3/2) exciton becomes Type-II and its intensity is only a few percent of the ground state Type-I σ+ (-1/2, -3/2) transition. Structures in which the upper σ- exciton is Type-II offer the possibility of hole spin-population inversion under optical pumping. The second structure studied (x=0.05, y=0.04) has a zero field valence band offset which is larger than the heavy hole saturation magnetic field splitting of the ZnCdMnSe layers. As a result, both σ+ and σ- transitions remain Type-I and their intensities are comparable. øbeylines ^1W.J. Walecki et. al, Appl. Phys. Lett. 57, 466 (1990). Supported by NSF, Grant No. DMR-9223054. ^**Supported by ONR.
NASA Astrophysics Data System (ADS)
Martucci, Mary B.
The field of spintronics, the development of spin-based devices that utilize the spin degree of freedom to increase memory capacity, has emerged as a solution to faster more efficient memory storage for electronic devices. One class of materials that has been extensively studied is the half-metallic ferromagnets, compounds that are 100% spin-polarized at the Fermi level. One material in this group that has been investigated is chromium telluride (Cr 1-xTe), whose family of compounds is known to exhibit a wide range of interesting magnetic and electronic properties. We have developed a hot injection solution synthesis of Cr5Te8 nanoplatlets which show similar magnetic behavior to the bulk material. It has also been shown that selenium and sulfur analogues can be obtained without changing the reaction conditions, making progress toward a better understanding of the reaction as well as an interesting family of compounds. Using real-space simulations, the effect of polarons in the high-Tc superconducting cuprates has been studied. The simulations demonstrate energetically favorable sites for the defects and show evidence of longer-range pairing interactions. Variations of the stripe show similar energetic results. X-ray absorption fine structure spectroscopy and neutron scattering have been utilized to examine the local structure of Ni-doped Mg nanoparticles, a hydrogen storage material as well as Cu2ZnSnS4 (CZTS) nanoparticles, a photovoltaic material. The Mg-Ni material shows much local disorder upon hydrogen cycling. The CZTS data demonstrate a loss of sulfur from around the copper sites upon annealing, helping to explain the changes observed in the optical absorption properties resulting from the annealing process.
Exciton-Exciton Interaction in KMnF3
NASA Astrophysics Data System (ADS)
Strauss, E.; Maniscalco, W. J.; Yen, W. M.; Kellner, U. C.; Gerhardt, V.
1980-03-01
Exciton dynamics in KMnF3 at exciton densities up to 1016 cm-3 are examined with time-resolved emission spectroscopy. The exciton emission line shifts and broadens with increasing exciton density. A nonlinear exciton decay channel is observed. These effects are found to be consistent with an exciton-exciton process. The shift scales with the exciton density and suggests that the effect is dominated by pairwise interactions up to the densities reached in these experiments.
Giant Optical Polarization Rotation Induced by Spin-Orbit Coupling in Polarons
NASA Astrophysics Data System (ADS)
Casals, Blai; Cichelero, Rafael; García Fernández, Pablo; Junquera, Javier; Pesquera, David; Campoy-Quiles, Mariano; Infante, Ingrid C.; Sánchez, Florencio; Fontcuberta, Josep; Herranz, Gervasi
2016-07-01
We have uncovered a giant gyrotropic magneto-optical response for doped ferromagnetic manganite La2 /3Ca1 /3MnO3 around the near room-temperature paramagnetic-to-ferromagnetic transition. At odds with current wisdom, where this response is usually assumed to be fundamentally fixed by the electronic band structure, we point to the presence of small polarons as the driving force for this unexpected phenomenon. We explain the observed properties by the intricate interplay of mobility, Jahn-Teller effect, and spin-orbit coupling of small polarons. As magnetic polarons are ubiquitously inherent to many strongly correlated systems, our results provide an original, general pathway towards the generation of magnetic-responsive gigantic gyrotropic responses that may open novel avenues for magnetoelectric coupling beyond the conventional modulation of magnetization.
Chiral topological excitons in the monolayer transition metal dichalcogenides.
Gong, Z R; Luo, W Z; Jiang, Z F; Fu, H C
2017-02-10
We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number = 2. The dependence of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength is numerically revealed. The chiral topological valley excitons are not only important to the excitonic transport due to prevention of the backscattering, but also give rise to the quantum coherent control in the optoelectronic applications.
Chiral topological excitons in the monolayer transition metal dichalcogenides
NASA Astrophysics Data System (ADS)
Gong, Z. R.; Luo, W. Z.; Jiang, Z. F.; Fu, H. C.
2017-02-01
We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number = 2. The dependence of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength is numerically revealed. The chiral topological valley excitons are not only important to the excitonic transport due to prevention of the backscattering, but also give rise to the quantum coherent control in the optoelectronic applications.
Chiral topological excitons in the monolayer transition metal dichalcogenides
Gong, Z. R.; Luo, W. Z.; Jiang, Z. F.; Fu, H. C.
2017-01-01
We theoretically investigate the chiral topological excitons emerging in the monolayer transition metal dichalcogenides, where a bulk energy gap of valley excitons is opened up by a position dependent external magnetic field. We find two emerging chiral topological nontrivial excitons states, which exactly connects to the bulk topological properties, i.e., Chern number = 2. The dependence of the spectrum of the chiral topological excitons on the width of the magnetic field domain wall as well as the magnetic filed strength is numerically revealed. The chiral topological valley excitons are not only important to the excitonic transport due to prevention of the backscattering, but also give rise to the quantum coherent control in the optoelectronic applications. PMID:28186154
Zarrabi, Nasim; Burn, Paul L; Meredith, Paul; Shaw, Paul E
2016-07-21
Transient absorption spectroscopy on organic semiconductor blends for solar cells typically shows efficient charge generation within ∼100 fs, accounting for the majority of the charge carriers. In this Letter, we show using transient absorption spectroscopy on blends containing a broad range of acceptor content (0.01-50% by weight) that the rise of the polaron signal is dependent on the acceptor concentration. For low acceptor content (<10% by weight), the polaron signal rises gradually over ∼1 ps with most polarons generated after 200 fs, while for higher acceptor concentrations (>10%) most polarons are generated within 200 fs. The rise time in blends with low acceptor content was also found to be sensitive to the pump fluence, decreasing with increasing excitation density. These results indicate that the sub-100 fs rise of the polaron signal is a natural consequence of both the high acceptor concentrations in many donor-acceptor blends and the high excitation densities needed for transient absorption spectroscopy, which results in a short average distance between the exciton and the donor-acceptor interface.
Excitons in the Fractional Quantum Hall Effect
DOE R&D Accomplishments Database
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.
Excitonic susceptibility in near triangular quantum wells
NASA Astrophysics Data System (ADS)
Anitha, A.; Arulmozhi, M.
2017-03-01
Diamagnetic susceptibility and binding energy of an exciton in a near triangular quantum well, with potential profile proportional to |z|2/3 composed of GaAs/Ga1- x Al x As and ZnO/Zn1- x Mg x O are calculated as a function of the wellwidth and concentration of Al and Mg respectively varying the magnetic field applied along growth direction (i.e. z-axis). Diamagnetic susceptibility of light hole exciton and heavy hole exciton, shows inverse behaviors in the two materials below 20 nm wellwidth and the binding energy of both excitons increases, as the magnetic field increases. The results obtained, are compared with those of quantum wells with varied potential profiles and the experimental results reported in the literature.
Theory of exciton transfer and diffusion in conjugated polymers
Barford, William; Tozer, Oliver Robert
2014-10-28
We describe a theory of Förster-type exciton transfer between conjugated polymers. The theory is built on three assumptions. First, we assume that the low-lying excited states of conjugated polymers are Frenkel excitons coupled to local normal modes, and described by the Frenkel-Holstein model. Second, we assume that the relevant parameter regime is ℏω < J, i.e., the adiabatic regime, and thus the Born-Oppenheimer factorization of the electronic and nuclear degrees of freedom is generally applicable. Finally, we assume that the Condon approximation is valid, i.e., the exciton-polaron wavefunction is essentially independent of the normal modes. The resulting expression for the exciton transfer rate has a familiar form, being a function of the exciton transfer integral and the effective Franck-Condon factors. The effective Franck-Condon factors are functions of the effective Huang-Rhys parameters, which are inversely proportional to the chromophore size. The Born-Oppenheimer expressions were checked against DMRG calculations, and are found to be within 10% of the exact value for a tiny fraction of the computational cost. This theory of exciton transfer is then applied to model exciton migration in conformationally disordered poly(p-phenylene vinylene). Key to this modeling is the assumption that the donor and acceptor chromophores are defined by local exciton ground states (LEGSs). Since LEGSs are readily determined by the exciton center-of-mass wavefunction, this theory provides a quantitative link between polymer conformation and exciton migration. Our Monte Carlo simulations indicate that the exciton diffusion length depends weakly on the conformation of the polymer, with the diffusion length increasing slightly as the chromophores became straighter and longer. This is largely a geometrical effect: longer and straighter chromophores extend over larger distances. The calculated diffusion lengths of ∼10 nm are in good agreement with experiment. The spectral
Optical and electronic properties of quantum dots with magnetic impurities
NASA Astrophysics Data System (ADS)
Govorov, Alexander O.
2008-10-01
The article discusses some of the recent results on semiconductor quantum dots with magnetic impurities. A single Mn impurity incorporated in a quantum dot strongly changes the optical response of a quantum-dot system. A character of Mn-carrier interaction is very different for II-VI and III-V quantum dots (QDs). In the II-VI QDs, a Mn impurity influences mostly the spin-structure of an exciton. In the III-V dots, a spatial localization of hole by a Mn impurity can be very important, and ultimately yields a totally different spin structure. A Mn-doped QD with a variable number of mobile carriers represents an artificial magnetic atom. Due to the Mn-carrier interaction, the order of filling of electronic shells in the magnetic QDs can be very different to the case of the real atoms. The "periodic" table of the artificial magnetic atoms can be realized in voltage-tunable transistor structures. For the electron numbers corresponding to the regime of Hund's rule, the magnetic Mn-carrier coupling is especially strong and the magnetic-polaron states are very robust. Magnetic QD molecules are also very different to the real molecules. QD molecules can demonstrate spontaneous breaking of symmetry and phase transitions. Single QDs and QD molecules can be viewed as voltage-tunable nanoscale memory cells where information is stored in the form of robust magnetic-polaron states. To cite this article: A.O. Govorov, C. R. Physique 9 (2008).
Exciton-phonon system on a star graph: A perturbative approach.
Yalouz, Saad; Pouthier, Vincent
2016-05-01
Based on the operatorial formulation of the perturbation theory, the properties of an exciton coupled with optical phonons on a star graph are investigated. Within this method, the dynamics is governed by an effective Hamiltonian, which accounts for exciton-phonon entanglement. The exciton is dressed by a virtual phonon cloud whereas the phonons are clothed by virtual excitonic transitions. In spite of the coupling with the phonons, it is shown that the energy spectrum of the dressed exciton resembles that of a bare exciton. The only differences originate in a polaronic mechanism that favors an energy shift and a decay of the exciton hopping constant. By contrast, the motion of the exciton allows the phonons to propagate over the graph so that the dressed normal modes drastically differ from the localized modes associated to bare phonons. They define extended vibrations whose properties depend on the state occupied by the exciton that accompanies the phonons. It is shown that the phonon frequencies, either red shifted or blue shifted, are very sensitive to the model parameter in general, and to the size of the graph in particular.
Exciton-phonon system on a star graph: A perturbative approach
NASA Astrophysics Data System (ADS)
Yalouz, Saad; Pouthier, Vincent
2016-05-01
Based on the operatorial formulation of the perturbation theory, the properties of an exciton coupled with optical phonons on a star graph are investigated. Within this method, the dynamics is governed by an effective Hamiltonian, which accounts for exciton-phonon entanglement. The exciton is dressed by a virtual phonon cloud whereas the phonons are clothed by virtual excitonic transitions. In spite of the coupling with the phonons, it is shown that the energy spectrum of the dressed exciton resembles that of a bare exciton. The only differences originate in a polaronic mechanism that favors an energy shift and a decay of the exciton hopping constant. By contrast, the motion of the exciton allows the phonons to propagate over the graph so that the dressed normal modes drastically differ from the localized modes associated to bare phonons. They define extended vibrations whose properties depend on the state occupied by the exciton that accompanies the phonons. It is shown that the phonon frequencies, either red shifted or blue shifted, are very sensitive to the model parameter in general, and to the size of the graph in particular.
Bose Polarons in the Strongly Interacting Regime
NASA Astrophysics Data System (ADS)
Hu, Ming-Guang; Van de Graaff, Michael J.; Kedar, Dhruv; Corson, John P.; Cornell, Eric A.; Jin, Deborah S.
2016-07-01
When an impurity is immersed in a Bose-Einstein condensate, impurity-boson interactions are expected to dress the impurity into a quasiparticle, the Bose polaron. We superimpose an ultracold atomic gas of 87Rb with a much lower density gas of fermionic 40 impurities. Through the use of a Feshbach resonance and radio-frequency spectroscopy, we characterize the energy, spectral width, and lifetime of the resultant polaron on both the attractive and the repulsive branches in the strongly interacting regime. The width of the polaron in the attractive branch is narrow compared to its binding energy, even as the two-body scattering length diverges.
Polarons and Mobile Impurities Near a Quantum Phase Transition
NASA Astrophysics Data System (ADS)
Shadkhoo, Shahriar
aforementioned polaronic and solitonic states. We eventually generalize the polaron formalism to the case of impurities that couple quadratically to a nearly-critical field; hence called the ''quadratic polaron''. The Hertz-Millis field theory and its generalization to the case of magnetic transition in helimagnets, is taken as a toy model. The phase diagram of the bare model contains both second-order and fluctuation-induced first-order quantum phase transitions. We propose a semi-classical scenario in which the impurity and the field couple quadratically. The polaron properties in the vicinity of these transitions are calculated in different dimensions. We observe that the quadratic coupling in three dimensions, even in the absence of the critical modes with finite wavelength, leads to a jump-like localization of the polaron. In lower dimensions, the transition behavior remains qualitatively similar to those in the case of linear coupling, namely the critical modes must have a finite wavelength to localize the particle.
Path-integral approach to lattice polarons
NASA Astrophysics Data System (ADS)
Kornilovitch, P. E.
2007-06-01
The basic principles behind a path integral approach to the lattice polaron are reviewed. Analytical integration of phonons reduces the problem to one self-interacting imaginary-time path, which is then simulated by Metropolis Monte Carlo. Projection operators separate states of different symmetry, which provides access to various excited states. Shifted boundary conditions in imaginary time enable calculation of the polaron mass, spectrum and density of states. Other polaron characteristics accessible by the method include the polaron energy, number of excited phonons and isotope exponent on mass. Monte Carlo updates are formulated in continuous imaginary time on infinite lattices and as such provide statistically unbiased results without finite-size and finite time-step errors. Numerical data are presented for models with short-range and long-range electron-phonon interactions.
Polaron action for multimode dispersive phonon systems
NASA Astrophysics Data System (ADS)
Kornilovitch, P. E.
2006-03-01
The path-integral approach to the tight-binding polaron is extended to multiple optical phonon modes of arbitrary dispersion and polarization. The nonlinear lattice effects are neglected. Only one electron band is considered. The electron-phonon interaction is of the density-displacement type, but can be of arbitrary spatial range and shape. Feynman’s analytical integration of ion trajectories is performed by transforming the electron-ion forces to the basis in which the phonon dynamical matrix is diagonal. The resulting polaron action is derived for the periodic and shifted boundary conditions in imaginary time. The former can be used for calculating polaron thermodynamics while the latter for the polaron mass and spectrum. The developed formalism is the analytical basis for numerical analysis of such models by path-integral Monte Carlo methods.
Small-polaron theory of doped antiferromagnets
NASA Astrophysics Data System (ADS)
Auerbach, Assa; Larson, Brond E.
1991-04-01
The spin-hole coherent-state path integral is used to generate a systematic large-spin expansion of the t-J model on the square lattice. The single hole's classical energy is minimized by small polarons with short-ranged interactions. Intersublattice hopping of polarons is forbidden by a tunneling selection rule. We derive the low-energy Lagrangian which reduces to the model of Wiegmann, Wen, Shankar, and Lee of Néel-gauge-field induced superconductivity.
Bose polarons in the strongly interacting regime
NASA Astrophysics Data System (ADS)
Kedar, Dhruv; Hu, Ming-Guang; van de Graaff, Michael; Corson, John; Cornell, Eric; Jin, Deborah
2016-05-01
Impurities immersed in and interacting with a Bose-Einstein condensate (BEC) are predicted to form quasiparticle excitations called Bose polarons. I will present experimental evidence of Bose polarons in cold atoms obtained using radio-frequency spectroscopy to measure the excitation spectrum of fermionic K-40 impurities interacting with a BEC of Rb-87 atoms. We use an interspecies Feshbach resonance to tune the interactions between the impurities and the bosons, and we take data in the strongly interacting regime.
Evidence for dark excitons in a single carbon nanotube due to the Aharonov-Bohm effect.
Matsunaga, Ryusuke; Matsuda, Kazunari; Kanemitsu, Yoshihiko
2008-10-03
We studied exciton structures and the Aharonov-Bohm effect in a single carbon nanotube using micro-photoluminescence (PL) spectroscopy under a magnetic field at low temperatures. A single sharp PL peak from the bright exciton state of a single carbon nanotube was observed under zero magnetic field, and the additional PL of dark exciton state appeared below the bright exciton peak under high magnetic fields. It was found that the split between the bright and dark exciton states is several millielectron volts at zero field. The tube diameter dependence of the splitting arises from the intervalley short-range Coulomb interaction.
Complex magneto-polaron spectrum of the layer compound InSe
NASA Astrophysics Data System (ADS)
Brancus, D. E. N.; Stan, G.; Dafinei, A.
2005-06-01
We analyse the energy magneto-polaron spectrum of the polar uniaxial layer compound InSe in a magnetic field directed along the optical axis. A quasi-bidimensional behaviour of the electron gas in this particular structure was considered. In the framework of the Wigner-Brillouin perturbational theory we systematically take into account all the sources of anisotropy. We found that the implied anisotropy brings distinctive contributions to the complex energy magneto-polaron spectrum of polar uniaxial crystals. The theory is used to examine the experimental results obtained from cyclotron resonance frequency measurements in InSe at low temperature.
The Holstein polaron problem revisited
NASA Astrophysics Data System (ADS)
Tayebi, Amin; Zelevinsky, Vladimir
2016-06-01
The Holstein Hamiltonian was proposed half a century ago; since then, decades of research have come up empty handed in the pursuit of a closed-form solution. An exact solution to the two-site Holstein model is presented in this paper. The obtained results provide a clear image of the Hamiltonian structure and allow for the investigation of the symmetry, energy level crossings and polaronic characteristics of the system. The main mathematical tool is a three-term recurrence relation between the wave function amplitudes, which was obtained using the properties of a family of orthogonal functions, namely the Poisson-Charlier polynomials. It is shown that, with the appropriate choice of basis, the eigenfunctions of the problem naturally fall into two families (parities) associated with the discrete {{{Z}}}2 symmetry of the Hamiltonian. The asymptotic solution to the recurrence relation is found by using the Birkhoff expansion. The asymptotic sets the truncation criterion for the wave function, which ensures the accurate calculation of the energy levels for any strength of electron-phonon interaction. The level crossing of states with different parities is discussed and the exact points of broken symmetry are found analytically. The results are used as the building blocks for studying a four-site system. The inherited symmetries lead to the formation of a sparse matrix that is convenient for numerical calculations.
Engineering Polarons at a Metal Oxide Surface
NASA Astrophysics Data System (ADS)
Yim, C. M.; Watkins, M. B.; Wolf, M. J.; Pang, C. L.; Hermansson, K.; Thornton, G.
2016-09-01
Polarons in metal oxides are important in processes such as catalysis, high temperature superconductivity, and dielectric breakdown in nanoscale electronics. Here, we study the behavior of electron small polarons associated with oxygen vacancies at rutile TiO2(110 ) , using a combination of low temperature scanning tunneling microscopy (STM), density functional theory, and classical molecular dynamics calculations. We find that the electrons are symmetrically distributed around isolated vacancies at 78 K, but as the temperature is reduced, their distributions become increasingly asymmetric, confirming their polaronic nature. By manipulating isolated vacancies with the STM tip, we show that particular configurations of polarons are preferred for given locations of the vacancies, which we ascribe to small residual electric fields in the surface. We also form a series of vacancy complexes and manipulate the Ti ions surrounding them, both of which change the associated electronic distributions. Thus, we demonstrate that the configurations of polarons can be engineered, paving the way for the construction of conductive pathways relevant to resistive switching devices.
Stationary Phonon Squeezing by Optical Polaron Excitation
NASA Astrophysics Data System (ADS)
Papenkort, T.; Axt, V. M.; Kuhn, T.
2017-03-01
We demonstrate that a stationary squeezed phonon state can be prepared by a pulsed optical excitation of a semiconductor quantum well. Unlike previously discussed scenarios for generating squeezed phonons, the corresponding uncertainties become stationary after the excitation and do not oscillate in time. The effect is caused by two-phonon correlations within the excited polaron. We demonstrate by quantum kinetic simulations and by a perturbation analysis that the energetically lowest polaron state comprises two-phonon correlations which, after the pulse, result in an uncertainty of the lattice momentum that is continuously lower than in the ground state of the semiconductor. The simulations show the dynamics of the polaron formation process and the resulting time-dependent lattice uncertainties.
Huber, Rachel C; Ferreira, Amy S; Thompson, Robert; Kilbride, Daniel; Knutson, Nicholas S; Devi, Lekshmi Sudha; Toso, Daniel B; Challa, J Reddy; Zhou, Z Hong; Rubin, Yves; Schwartz, Benjamin J; Tolbert, Sarah H
2015-06-19
The efficiency of biological photosynthesis results from the exquisite organization of photoactive elements that promote rapid movement of charge carriers out of a critical recombination range. If synthetic organic photovoltaic materials could mimic this assembly, charge separation and collection could be markedly enhanced. We show that micelle-forming cationic semiconducting polymers can coassemble in water with cationic fullerene derivatives to create photoinduced electron-transfer cascades that lead to exceptionally long-lived polarons. The stability of the polarons depends on the organization of the polymer-fullerene assembly. Properly designed assemblies can produce separated polaronic charges that are stable for days or weeks in aqueous solution.
Spin-exciton interaction and related micro-photoluminescence spectra of ZnSe:Mn DMS nanoribbon.
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.
The asymmetric quantum Rabi model in the polaron picture
NASA Astrophysics Data System (ADS)
Liu, Maoxin; Ying, Zu-Jian; An, Jun-Hong; Luo, Hong-Gang; Lin, Hai-Qin
2017-02-01
The concept of the polaron in condensed matter physics has been extended to the Rabi model, where polarons resulting from the coupling between a two-level system and single-mode photons represent two oppositely displaced oscillators. Interestingly, tunneling between these two displaced oscillators can induce an anti-polaron, which has not been systematically explored in the literature, especially in the presence of an asymmetric term. In this paper, we present a systematic analysis of the competition between the polaron and anti-polaron under the interplay of the coupling strength and the asymmetric term. While intuitively the anti-polaron should be secondary owing to its higher potential energy, we find that, under certain conditions, the minor anti-polaron may gain a reversal in the weight over the major polaron. If the asymmetric amplitude ɛ is smaller than the harmonic frequency ω, such an overweighted anti-polaron can occur beyond a critical value of the coupling strength g; if ɛ is larger, the anti-polaron can even be always overweighted at any g. We propose that the explicit occurrence of the overweighted anti-polaron can be monitored by a displacement transition from negative to positive values. This displacement is an experimentally accessible observable, which can be measured by quantum optical methods, such as balanced Homodyne detection.
Dynamical frustration versus kinetic enhancement with excitons in strongly correlated bilayers
NASA Astrophysics Data System (ADS)
Rademaker, Louk
2014-03-01
Recently the condensation of electron-hole pairs in semiconductor bilayers has been achieved. This has opened up the pursuit of exciton condensation in other layered materials. Here I will present recent theoretical work on exciton physics in complex oxide heterostructures. The poorly understood high temperature superconducting cuprates are ideal candidates for bilayer exciton condensation. Therefore we study the dynamics and the phase diagram of bilayer excitons in a Mott insulating p/n heterostructure, which shows rich exciton-spin interaction phenomena. I will discuss the dynamical frustration experienced by an exciton moving through an antiferromagnetic background. In sharp contrast, I will show how in the exciton superfluid phase the magnetic excitations 'borrow' kinetic energy from the excitons.
Electrons on helium — The ``polaron'' transition
NASA Astrophysics Data System (ADS)
Andrei, E. Y.; Grimes, C. C.; Adams, G.
1984-07-01
We describe the observation of the polaronic transition of a system of electrons supported above a helium film. The electron mobility drops sharply by more than four orders of magnitude as the film thickness is reduced below ≈ 1000 Å. The transition was observed in the temperature range 0.4 ⩽ T ⩽ 1 K.
Coherent state polarons in quantum wells
NASA Astrophysics Data System (ADS)
Thilagam, A.; Lohe, M. A.
2005-01-01
We investigate the polaronic effects of an electron confined in a quantum well, which we describe through its algebraic properties using su (1 , 1), taking into account the electron-bulk longitudinal-optical phonon interaction. We construct the variational wave function as the direct product of an electronic part and a part describing coherent phonons generated by the Low-Lee-Pines transformation from the vacuum state. We use two explicit forms of coherent states, Perelomov and Barut-Girardello states, to represent the electronic part in the quantum well spectrum. Our results show that in a coherent state basis for electrons the basic polaron parameters such as the energy gap shift and effective mass are further enhanced compared to those obtained with the conventional sinusoidal form of the basis. The difference between the two types of quantum well coherent states appears in polaronic interactions in quantum wells. We extend the calculations in order to estimate polaron lifetimes for a variety of different material systems.
Control of exciton fluxes in an excitonic integrated circuit.
High, Alex A; Novitskaya, Ekaterina E; Butov, Leonid V; Hanson, Micah; Gossard, Arthur C
2008-07-11
Efficient signal communication uses photons. Signal processing, however, uses an optically inactive medium, electrons. Therefore, an interconnection between electronic signal processing and optical communication is required at the integrated circuit level. We demonstrated control of exciton fluxes in an excitonic integrated circuit. The circuit consists of three exciton optoelectronic transistors and performs operations with exciton fluxes, such as directional switching and merging. Photons transform into excitons at the circuit input, and the excitons transform into photons at the circuit output. The exciton flux from the input to the output is controlled by a pattern of the electrode voltages. The direct coupling of photons, used in communication, to excitons, used as the device-operation medium, may lead to the development of efficient exciton-based optoelectronic devices.
Polarons and bipolarons in cis-polyacetylene
NASA Astrophysics Data System (ADS)
Utz, Wolfram; Förner, Wolfgang
1998-05-01
We present a parametrization for the Pariser-Parr-Pople Hamiltonian for the description of cis-polyacetylene (cPA). In contrast to trans-polyacetylene, we have to include symmetry breaking between neighboring sites into the Su-Schrieffer-Heeger-type one-electron part of the Hamiltonian. Our parametrization is based on correlated ab initio calculations on cis-hexatriene and on the results of independent calculations found in the literature. For open-shell systems (singly charged polarons) we use the annihilated unrestricted Hartree-Fock method to avoid the artificial spin contaminations inherent in UHF (unrestricted HF) calculations, which lead to the inclusion of fractions of the correlation energy in UHF total energies which cannot be controlled and are different for different systems and even for different geometries of the same system. Thus UHF is useless for the calculation of potential hypersurfaces and thus in turn for dynamical simulations. We find that in cPA singly-charged polarons are formed, while in doubly-charged chains stable bipolarons are found, although of a quite large width. This is in contrast to recent results reported by Shimoi and Abe [Y. Shimoi and S. Abe, Synth. Met. 69, 687 (1995) and Phys. Rev. B 50, 14 781 (1994)] who found that two singly-charged polarons are more stable for realistic parameter values than a doubly-charged bipolaron. We further find that the charged polarons are mobile in the chain and thus we conclude that polarons and bipolarons can serve as charge carriers (the latter ones spinless) in doped cPA.
NASA Astrophysics Data System (ADS)
Zhao, Guo-Meng
2007-07-01
A penetration depth measurement was carried out on the optimally doped bismuthate superconductor Ba0.63K0.37BiO3 (Tc=29.2K) using the muon-spin-relaxation technique. We find that the temperature dependence of the penetration depth λ(T) of this compound is in excellent agreement with strong-coupling phonon-mediated superconductivity with a reduced energy gap of 2Δ(0)/kBTc=4.4 and a retarded electron-phonon coupling constant λe-p=1.4 . The observed large reduced energy gap rules out the possibility of pairing mechanisms based on coupling to high-energy electronic excitations. Quantitative data analyses indicate that high-temperature superconductivity in bismuthates arises from the Cooper pairing of polaronic charge carriers.
NASA Astrophysics Data System (ADS)
Astakhov, G. V.; Yakovlev, D. R.; Crooker, S. A.; Ossau, W.; Christianen, P. C. M.; Rudenkov, V. V.; Karczewski, G.; Wojtowicz, T.; Kossut, J.
2004-02-01
We present comprehensive study of negatively charged exciton in high magnetic fields for filling factors < 1. In magneto-optical spectra the fine structure was found to be contributed by neutral exciton and different a set of bound states of charged exciton. These states were identified due to their unique polarization properties charecteristics in emission and absorption spectra.
Bose polarons: Dynamical decay and RF signatures
NASA Astrophysics Data System (ADS)
Corson, John; Bohn, John
2016-05-01
Interactions of a single impurity with a quantum many-body environment are known to alter the character of the impurity, thereby forming a ``quasiparticle''. The condensed matter tradition often identifies quasiparticles as poles of a Green function in the complex plane, a notion whose sophistication sometimes obscures the underlying physics. The problem of a single quantum impurity in a Bose condensate, or Bose polaron, is an illustrative example where the meaning of the impurity Green function, and hence the quasiparticle itself, becomes especially transparent. Using direct diagonalization in a truncated Hilbert space, we examine the dynamical evolution and quasiparticle decay of the repulsive Bose polaron. This approach also allows us to simulate RF spectroscopy across a Feshbach resonance and outside the linear regime, as well as account for motional and thermal effects in a harmonic trap.
Possible formation of chiral polarons in graphene.
Kandemir, B S
2013-01-16
A theoretical investigation of the possible existence of chiral polaron formation in graphene is reported. We present an analytical method to calculate the ground-state of the electron-phonon system within the framework of the Lee-Low-Pines theory. On the basis of our model, the influence of electron-optical phonon interaction on the graphene electronic spectrum is investigated. We considered only the doubly degenerate optical phonon modes of E(2g) symmetry near the zone center Γ. It is analytically shown that the energy dispersions of both valence and conduction bands of the pristine graphene differ significantly from those obtained through the standard electron self-energy calculations arising from the electron-optical phonon interactions. In this paper, we also show for the first time that the degenerate band structure of the graphene promotes the chiral polaron formation. Furthermore, due to the k-dependent nature of the polaronic self-energy, in analogy with quantum chromodynamics, we also propose a running electron-phonon coupling constant as a function of energy.
Polaron dynamics in anisotropic Holstein-Peierls systems.
Ribeiro Junior, Luiz Antonio; Stafström, Sven
2017-02-01
Polaron dynamics in anisotropic organic molecular semiconductors is theoretically investigated and simulated in the framework of a semi-classical Holstein-Peierls model. Our computational protocol is presented and applied to studies of a two-dimensional molecular crystal. The intermolecular (Peierls) parameters for a particular crystal direction are systematically changed in order to study the effect of anisotropy in the system. The usefulness of this methodology is highlighted by studying the polaron dynamics on a picosecond timescale, which provides a microscopic insight into the influence of the interplay between different intramolecular parameters on the charge transport mechanism. Our results show that the polaron mobility is substantially reduced in going from an anisotropic to an isotropic relationship between the Peierls parameters for different directions in the crystal. Interestingly, the molecular charge distribution presents three different signatures corresponding to a one-dimensional polaron, a two-dimensional polaron, and an intermediate state for which the polaron localization depends on the degree of anisotropy. Importantly, the two-dimensional polaron, which is present in the essentially isotropic system, is immobile whereas the other two types of polarons are mobile. This, in order for polaron transport to occur in a two-dimensional molecular based system, this system has to be anisotropic.
Crooker, S. A.; Kelley, M. R.; Martinez, N. J. D.; Nie, W.; Mohite, A.; Nayyar, I. H.; Tretiak, S.; Smith, D. L.; Liu, F.; Ruden, P. P.
2014-10-13
We use spectrally resolved magneto-electroluminescence (EL) measurements to study the energy dependence of hyperfine interactions between polaron and nuclear spins in organic light-emitting diodes. Using layered devices that generate bright exciplex emission, we show that the increase in EL emission intensity I due to small applied magnetic fields of order 100 mT is markedly larger at the high-energy blue end of the EL spectrum (ΔI/I ∼ 11%) than at the low-energy red end (∼4%). Concurrently, the widths of the magneto-EL curves increase monotonically from blue to red, revealing an increasing hyperfine coupling between polarons and nuclei and directly providing insight into the energy-dependent spatial extent and localization of polarons.
Energy levels of magneto-optical polaron in spherical quantum dot — Part 1: Strong coupling
NASA Astrophysics Data System (ADS)
Fotue, A. J.; Kenfack, S. C.; Issofa, N.; Tiotsop, M.; Fotsin, H.; Mainimo, E.; Fai, L. C.
2015-09-01
We investigate the influence of a magnetic field on the ground state energy of a polaron in a spherical semiconductor quantum dot (QD) using the modified LLP method. The ground state energy is split into sub-energy levels and there is a degeneracy of energy levels. It is also observed that the degenerate energy increase with the electron-phonon coupling constant and decrease with the magnetic field. The numerical results show that, under the influence of magnetic field and the interaction with the total momentum along the z-direction, the split energy increases and decreases with the longitudinal and the transverse confinement length, respectively.
Spin–exciton interaction and related micro-photoluminescence spectra of ZnSe:Mn DMS nanoribbon
NASA Astrophysics Data System (ADS)
Hou, Lipeng; Zhou, Weichang; Zou, Bingsuo; Zhang, Yu; Han, Junbo; Yang, Xinxin; Gong, Zhihong; Li, Jingbo; Xie, Sishen; Shi, Li-Jie
2017-03-01
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 Mn2+–Mn2+ 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.
Permanent Rabi oscillations in coupled exciton-photon systems with PT-symmetry.
Chestnov, Igor Yu; Demirchyan, Sevak S; Alodjants, Alexander P; Rubo, Yuri G; Kavokin, Alexey V
2016-01-21
We propose a physical mechanism which enables permanent Rabi oscillations in driven-dissipative condensates of exciton-polaritons in semiconductor microcavities subjected to external magnetic fields. The method is based on stimulated scattering of excitons from the incoherent reservoir. We demonstrate that permanent non-decaying oscillations may appear due to the parity-time symmetry of the coupled exciton-photon system realized in a specific regime of pumping to the exciton state and depletion of the reservoir. At non-zero exciton-photon detuning, robust permanent Rabi oscillations occur with unequal amplitudes of exciton and photon components. Our predictions pave way to realization of integrated circuits based on exciton-polariton Rabi oscillators.
Permanent Rabi oscillations in coupled exciton-photon systems with PT -symmetry
Chestnov, Igor Yu.; Demirchyan, Sevak S.; Alodjants, Alexander P.; Rubo, Yuri G.; Kavokin, Alexey V.
2016-01-01
We propose a physical mechanism which enables permanent Rabi oscillations in driven-dissipative condensates of exciton-polaritons in semiconductor microcavities subjected to external magnetic fields. The method is based on stimulated scattering of excitons from the incoherent reservoir. We demonstrate that permanent non-decaying oscillations may appear due to the parity-time symmetry of the coupled exciton-photon system realized in a specific regime of pumping to the exciton state and depletion of the reservoir. At non-zero exciton-photon detuning, robust permanent Rabi oscillations occur with unequal amplitudes of exciton and photon components. Our predictions pave way to realization of integrated circuits based on exciton-polariton Rabi oscillators. PMID:26790534
NASA Astrophysics Data System (ADS)
Lioudakis, Emmanouil; Alexandrou, Ioannis; Othonos, Andreas
2009-12-01
Nowadays, organic solar cells have the interest of engineers for manufacturing flexible and low cost devices. The considerable progress of this nanotechnology area presents the possibility of investigating new effects from a fundamental science point of view. In this letter we highlight the influence of the concentration of fullerene molecules on the ultrafast transport properties of charged electrons and polarons in P3HT/PCBM blended materials which are crucial for the development of organic solar cells. Especially, we report on the femtosecond dynamics of localized (P2 at 1.45 eV) and delocalized (DP2 at 1.76 eV) polaron states of P3HT matrix with the addition of fullerene molecules as well as the free-electron relaxation dynamics of PCBM-related states. Our study shows that as PCBM concentration increases, the amplified exciton dissociation at bulk heterojunctions leads to increased polaron lifetimes. However, the increase in PCBM concentration can be directly related to the localization of polarons, creating thus two competing trends within the material. Our methodology shows that the effect of changes in structure and/or composition can be monitored at the fundamental level toward optimization of device efficiency.
electric dipole superconductor in bilayer exciton system
NASA Astrophysics Data System (ADS)
Sun, Qing-Feng; Jiang, Qing-Dong; Bao, Zhi-Qiang; Xie, X. C.
Recently, it was reported that the bilayer exciton systems could exhibit many new phenomena, including the large bilayer counterflow conductivity, the Coulomb drag, etc. These phenomena imply the formation of exciton condensate superfluid state. On the other hand, it is now well known that the superconductor is the condensate superfluid state of the Cooper pairs, which can be viewed as electric monopoles. In other words, the superconductor state is the electric monopole condensate superfluid state. Thus, one may wonder whether there exists electric dipole superfluid state. In this talk, we point out that the exciton in a bilayer system can be considered as a charge neutral electric dipole. And we derive the London-type and Ginzburg-Landau-type equations of electric dipole superconductivity. From these equations, we discover the Meissner-type effect (against spatial variation of magnetic fields), and the dipole current Josephson effect. The frequency in the AC Josephson effect of the dipole current is equal to that in the normal (monopole) superconductor. These results can provide direct evidence for the formation of exciton superfluid state in the bilayer systems and pave new ways to obtain the electric dipole current. We gratefully acknowledge the financial support by NBRP of China (2012CB921303 and 2015CB921102) and NSF-China under Grants Nos. 11274364 and 11574007.
Diamagnetic excitons in semiconductors (Review)
NASA Astrophysics Data System (ADS)
Seisyan, R. P.
2016-05-01
Optical properties of semiconductor crystals in the presence of a high magnetic field have been considered. The field turn-on gives rise to oscillations of the optical-absorption edge or, more specifically, the formation of a complex absorption spectrum with a periodic structure, referred to as the spectrum of "diamagnetic excitons." Such spectra appear a source of the most accurate knowledge about the band structure of semiconductors. Moreover, these spectra can be used for simulating the low-dimensional state in semiconductors and possible interpretation of the emission spectra of neutron stars. The proposed analytical review is based on extensive experimental and theoretical data contained mostly in cited original works of the author with colleagues.
Artificially Constructed Plasmarons and Plasmon-Exciton Molecules in 2D Metals
NASA Astrophysics Data System (ADS)
Zhuravlev, A. S.; Kuznetsov, V. A.; Kulik, L. V.; Bisti, V. E.; Kirpichev, V. E.; Kukushkin, I. V.; Schmult, S.
2016-11-01
Resonant optical excitation was used to create a macroscopic nonequilibrium ensemble of "dark" excitons with an unprecedented long lifetime in a two-dimensional electron system placed in a quantizing magnetic field. Exotic three-particle and four-particle states, plasmarons and plasmon-exciton molecules, coupled with the surrounding electrons through the collective plasma oscillations are engineered. Plasmarons and plasmon-exciton molecules are manifested as new features in the recombination spectra of nonequilibrium systems.
Dual coupling effective band model for polarons
NASA Astrophysics Data System (ADS)
Marchand, Dominic J. J.; Stamp, Philip C. E.; Berciu, Mona
2017-01-01
Nondiagonal couplings to a bosonic bath completely change polaronic dynamics, from the usual diagonally coupled paradigm of smoothly varying properties. We study, using analytic and numerical methods, a model having both diagonal Holstein and nondiagonal Su-Schrieffer-Heeger (SSH) couplings. The critical coupling found previously in the pure SSH model, at which the k =0 effective mass diverges, now becomes a transition line in the coupling constant plane—the form of the line depends on the adiabaticity parameter. Detailed results are given for the quasiparticle and ground-state properties, over a wide range of couplings and adiabaticity ratios. The new paradigm involves a destabilization, at the transition line, of the simple Holstein polaron to one with a finite ground-state momentum, but with everywhere a continuously evolving band shape. No "self-trapping transition" exists in any of these models. The physics may be understood entirely in terms of competition between different hopping terms in a simple renormalized effective band theory. The possibility of further transitions is suggested by the results.
Doping dependent evolution of the polaron metal
NASA Astrophysics Data System (ADS)
Mannella, N.; Tanaka, K.; Mo, S.-K.; Yang, W.; Zheng, H.; Mitchell, J.; Zaanen, J.; Deveraux, T. P.; Nagaosa, N.; Hussain, Z.; Shen, Z.-X.
2009-03-01
Experimental and theoretical evidence has already suggested that the ferromagnetic metallic (FM) phase in colossal magnetoresistive manganites is not a conventional metal but rather a polaronic conductor. In the bilayer manganites La2-2xSr1+2xMn2O7 (LSMO), Angle Resolved Photoemission (ARPES) experiment revealed that the FM phase is a polaronic metal with a strong anisotropic character of the electronic excitations [1,2]. A small but well-defined quasiparticle (QP) with heavy mass along the [110] or ``nodal'' direction is found to account for the metallic properties and their temperature dependent evolution [2]. In this talk, we will discuss recent ARPES results on the x = 0.60 composition and contrast them to the x = 0.40 results. Recent work has shown that the region in proximity of x = 0.60 constitute the most metallic bilayer manganite with DC conductivity about one order of magnitude higher than that corresponding to the region 0.30 < x < 0.40. Much as in the x = 0.40 composition, for x = 0.60 along the nodal direction we observe a peak-dip-hump structure with QP of heavy effective mass. Quantitative differences in the electron-phonon coupling constant λ, the QP spectral weight and the hump energy are fully consistent with the doping evolution of the transport properties. [1] Nature 438, 474 (2005), [2] Phys. Rev. B 76, 233102 (2007).
Exciton storage in a nanoscale Aharonov-Bohm ring with electric field tuning.
Fischer, Andrea M; Campo, Vivaldo L; Portnoi, Mikhail E; Römer, Rudolf A
2009-03-06
We study analytically the optical properties of a simple model for an electron-hole pair on a ring subjected to perpendicular magnetic flux and in-plane electric field. We show how to tune this excitonic system from optically active to optically dark as a function of these external fields. Our results offer a simple mechanism for exciton storage and readout.
Exciton Storage in a Nanoscale Aharonov-Bohm Ring with Electric Field Tuning
Fischer, Andrea M.; Roemer, Rudolf A.; Campo, Vivaldo L. Jr.; Portnoi, Mikhail E.
2009-03-06
We study analytically the optical properties of a simple model for an electron-hole pair on a ring subjected to perpendicular magnetic flux and in-plane electric field. We show how to tune this excitonic system from optically active to optically dark as a function of these external fields. Our results offer a simple mechanism for exciton storage and readout.
Method of time-ordered products in polaron theory
Bogolyupov, N.N.; Kireev, A.N.; Kurbatov, A.M.
1986-10-01
The method of time-ordered products is used to investigate the equilibrium thermodynamic properties of the Frolich model in polaron theory. The polaron free energy at finite temperatures is calculated on the basis of Bogolyubov's variational principle. The trial functional is chosen in the most general form corresponding to an arbitrary number of harmonic oscillators interacting with the electron. An upper bound for the polaron ground-state energy is obtained and studied in the case of weak coupling and low temperatures. It is shown that the accuracy of the bound increases with increasing number of oscillators.
Small hole polarons in rare-earth titanates
Bjaalie, L.; Moetakef, P.; Cain, T. A.; Janotti, A.; Himmetoglu, B.; Stemmer, S.; Van de Walle, C. G.; Ouellette, D. G.; Allen, S. J.
2015-06-08
We investigate the behavior of hole polarons in rare-earth titanates by combining optical conductivity measurements with first-principles hybrid density functional calculations. Sr-doped GdTiO{sub 3} (Gd{sub 1−x}Sr{sub x}TiO{sub 3}) was grown by molecular beam epitaxy. We show that a feature in the optical conductivity that was previously identified with the Mott-Hubbard gap is actually associated with the excitation of a small polaron. The assignment is based on an excellent match between the experimental spectra and first-principles calculations for polaron excitation mechanisms.
Small polaron formation in porous WO3-x nanoparticle films
NASA Astrophysics Data System (ADS)
Ederth, J.; Hoel, A.; Niklasson, G. A.; Granqvist, C. G.
2004-11-01
Porous tungsten oxide nanoparticle films were prepared by reactive gas evaporation. The structure was studied by x-ray diffraction and scanning electron microscopy, and the oxygen nonstoichiometry was inferred by x-ray photoelectron spectroscopy, elastic recoil detection analysis, and neutron scattering. Specifically, the films consisted of WO3-x with 0.25
Quantum Dynamics of Ultracold Bose Polarons
NASA Astrophysics Data System (ADS)
Shchadilova, Yulia E.; Schmidt, Richard; Grusdt, Fabian; Demler, Eugene
2016-09-01
We analyze the dynamics of Bose polarons in the vicinity of a Feshbach resonance between the impurity and host atoms. We compute the radio-frequency absorption spectra for the case when the initial state of the impurity is noninteracting and the final state is strongly interacting with the host atoms. We compare results of different theoretical approaches including a single excitation expansion, a self-consistent T -matrix method, and a time-dependent coherent state approach. Our analysis reveals sharp spectral features arising from metastable states with several Bogoliubov excitations bound to the impurity atom. This surprising result of the interplay of many-body and few-body Efimov type bound state physics can only be obtained by going beyond the commonly used Fröhlich model and including quasiparticle scattering processes. Close to the resonance we find that strong fluctuations lead to a broad, incoherent absorption spectrum where no quasiparticle peak can be assigned.
Extreme electron polaron spatial delocalization in π-conjugated materials
Rawson, Jeff; Angiolillo, Paul J.; Therien, Michael J.
2015-01-01
The electron polaron, a spin-1/2 excitation, is the fundamental negative charge carrier in π-conjugated organic materials. Large polaron spatial dimensions result from weak electron-lattice coupling and thus identify materials with unusually low barriers for the charge transfer reactions that are central to electronic device applications. Here we demonstrate electron polarons in π-conjugated multiporphyrin arrays that feature vast areal delocalization. This finding is evidenced by concurrent optical and electron spin resonance measurements, coupled with electronic structure calculations that suggest atypically small reorganization energies for one-electron reduction of these materials. Because the electron polaron dimension can be linked to key performance metrics in organic photovoltaics, light-emitting diodes, and a host of other devices, these findings identify conjugated materials with exceptional optical, electronic, and spintronic properties. PMID:26512097
Polaronic interactions between oxygen vacancies in rutile Ti O2
NASA Astrophysics Data System (ADS)
Zhao, Liang; Magyari-Köpe, Blanka; Nishi, Yoshio
2017-02-01
Oxygen vacancy-vacancy interactions in rutile Ti O2 are studied in conjunction with polaron formation trends using density functional theory calculations. It is found that polarons strongly enhance the formation of oxygen vacancies in this material and also mediate the interactions between existing vacancies. At distances below 1 nm, two isolated and charge-neutral vacancies exhibit attractive interactions with an equilibrium distance of about 4 Å. The attractive forces between vacancies partly arise from the polaronic transfer of excess electrons to reduce the potential energy. These discoveries provide microscopic explanations to the vacancy clustering phenomena, as well as a practical approach to stabilize the polarons at arbitrary Ti atoms in Ti O2 .
Optical nonlinearities of small polarons in lithium niobate
NASA Astrophysics Data System (ADS)
Imlau, Mirco; Badorreck, Holger; Merschjann, Christoph
2015-12-01
An overview of optical nonlinearities of small bound polarons is given, which can occur in the congruently melting composition of LiNbO3. Such polarons decisively influence the linear and nonlinear optical performance of this material that is important for the field of optics and photonics. On the basis of an elementary phenomenological approach, the localization of carriers in a periodic lattice with intrinsic defects is introduced. It is applied to describe the binding energies of four electron and hole small polarons in LiNbO3: small free NbNb4 + polarons, small bound NbLi4 + polarons, small bound NbLi4 +:NbNb4 + bipolarons, and small bound O- hole polarons. For the understanding of their linear interaction with light, an optically induced transfer between nearest-neighboring polaronic sites is assumed. It reveals spectrally well separated optical absorption features in the visible and near-infrared spectral range, their small polaron peak energies and lineshapes. Nonlinear interaction of light is assigned to the optical formation of short-lived small polarons as a result of carrier excitation by means of band-to-band transitions. It is accompanied by the appearance of a transient absorption being spectrally constituted by the individual fingerprints of the small polarons involved. The relaxation dynamics of the transients is thermally activated and characterized phenomenologically by a stretched exponential behavior, according to incoherent 3D small polaron hopping between regular and defect sites of the crystal lattice. It is shown that the analysis of the dynamics is a useful tool for revealing the recombination processes between small polarons of different charge. Nonlinear interaction of small polarons with light furthermore results in changes of the index of refraction. Besides its causal relation to the transients via Kramers-Kronig relation, pronounced index changes may occur due to optically generated electric fields modulating the index of refraction
Tunable Polaronic Conduction in Anatase TiO2
NASA Astrophysics Data System (ADS)
Moser, S.; Moreschini, L.; Jaćimović, J.; Barišić, O. S.; Berger, H.; Magrez, A.; Chang, Y. J.; Kim, K. S.; Bostwick, A.; Rotenberg, E.; Forró, L.; Grioni, M.
2013-05-01
Oxygen vacancies created in anatase TiO2 by UV photons (80-130 eV) provide an effective electron-doping mechanism and induce a hitherto unobserved dispersive metallic state. Angle resolved photoemission reveals that the quasiparticles are large polarons. These results indicate that anatase can be tuned from an insulator to a polaron gas to a weakly correlated metal as a function of doping and clarify the nature of conductivity in this material.
Polaron formation and transport in olivine cathode materials
NASA Astrophysics Data System (ADS)
Johannes, Michelle; Hoang, Khang
2011-03-01
One of the critical factors limiting Li ion battery performance is electronic conduction through the cathode material. In the olivine structure type materials, such as LiFe PO4 , the parent materials are insulators with a gap of approximately 4 (or more) eV. The withdrawal of an electron results not in a band-type hole state, but rather a localized polaronic state. Transport then occurs via hopping of the polaron through the crystal. The measured electronic conduction in olivine materials depends on the transition metal cation type. In this study, we use density functional theory to compare formation of polarons in olivine materials with different transition metal cations: Mn, Fe, Co, and Ni. We show that the underlying electronic structure of the fully lithiated material (or fully delithiated material) essentially determines whether or not polaron formation is possible in localized d -states or whether the holes that result from adding or removing an electron reside in oxygen-derived states. We also investigate the facility of polaronic hopping by calculating the barrier between adjacent polaron sites in each of the four materials.
NASA Astrophysics Data System (ADS)
Zhang, Qi; Gao, Weilu; Watson, John; Manfra, Michael; Kono, Junichiro
2015-03-01
Density-dependent Coulomb interactions can drive electron-hole (e - h) pairs in semiconductors through an excitonic Mott transition from an excitonic gas into an e - h plasma. Theoretical studies suggest that these interactions can be strongly modified by an external magnetic field, including the absence of inter-exciton interactions in the high magnetic field limit in two dimensions, due to an e - h charge symmetry, which results in ultrastable magneto-excitons. Here, we present a systematic experimental study of e - h pairs in photo-excited undoped GaAs quantum wells in magnetic fields with ultrafast terahertz spectroscopy. We simultaneously monitored the dynamics of the intraexcitonic 1 s-2 p transition (which splits into 1 s-2p+ and 1 s-2p- transitions in a magnetic field) and the cyclotron resonance of unbound electrons and holes up to 10 Tesla. We found that the 1 s-2p- absorption feature is robust at high magnetic fields even under high excitation fluences, indicating magnetically enhanced stability of excitons. We will discuss the Mott physics of magneto-excitons as a function of temperature, e - h pair density, optical pump delay time, as well as magnetic field, and also compare two-dimensional excitons in GaAs quantum wells with three-dimensional excitons in bulk GaAs.
NASA Astrophysics Data System (ADS)
Ishii, A.; Yoshida, M.; Kato, Y. K.
2015-03-01
Luminescence properties of carbon nanotubes are strongly affected by exciton diffusion, which plays an important role in various nonradiative decay processes. Here we perform photoluminescence microscopy on hundreds of individual air-suspended carbon nanotubes to elucidate the interplay between exciton diffusion, end quenching, and exciton-exciton annihilation processes. A model derived from random-walk theory as well as Monte Carlo simulations are utilized to analyze nanotube length dependence and excitation power dependence of emission intensity. We have obtained the values of exciton diffusion length and absorption cross section for different chiralities, and diameter-dependent photoluminescence quantum yields have been observed. The simulations have also revealed the nature of a one-dimensional coalescence process, and an analytical expression for the power dependence of emission intensity is given.
Exciton-photon correlations in bosonic condensates of exciton-polaritons.
Kavokin, Alexey V; Sheremet, Alexandra S; Shelykh, Ivan A; Lagoudakis, Pavlos G; Rubo, Yuri G
2015-07-08
Exciton-polaritons are mixed light-matter quasiparticles. We have developed a statistical model describing stochastic exciton-photon transitions within a condensate of exciton polaritons. We show that the exciton-photon correlator depends on the rate of incoherent exciton-photon transformations in the condensate. We discuss implications of this effect for the quantum statistics of photons emitted by polariton lasers.
Ulbricht, Ronald; Pijpers, Joep J H; Groeneveld, Esther; Koole, Rolf; Donega, Celso de Mello; Vanmaekelbergh, Daniel; Delerue, Christophe; Allan, Guy; Bonn, Mischa
2012-09-12
We report on the gradual evolution of the conductivity of spherical CdTe nanocrystals of increasing size from the regime of strong quantum confinement with truly discrete energy levels to the regime of weak confinement with closely spaced hole states. We use the high-frequency (terahertz) real and imaginary conductivities of optically injected carriers in the nanocrystals to report on the degree of quantum confinement. For the smaller CdTe nanocrystals (3 nm < radius < 5 nm), the complex terahertz conductivity is purely imaginary. For nanocrystals with radii exceeding 5 nm, we observe the onset of real conductivity, which is attributed to the increasingly smaller separation between the hole states. Remarkably, this onset occurs for a nanocrystal radius significantly smaller than the bulk exciton Bohr radius a(B) ∼ 7 nm and cannot be explained by purely electronic transitions between hole states, as evidenced by tight-binding calculations. The real-valued conductivity observed in the larger nanocrystals can be explained by the emergence of mixed carrier-phonon, that is, polaron, states due to hole transitions that become resonant with, and couple strongly to, optical phonon modes for larger QDs. These polaron states possess larger oscillator strengths and broader absorption, and thereby give rise to enhanced real conductivity within the nanocrystals despite the confinement.
Transient Exciton Spin Splitting in GaAs Quantum Wells under Near-Resonant Excitation
NASA Astrophysics Data System (ADS)
Zin Latt, Kyaw; Lai, Chih-Wei
2010-03-01
We investigated spin dependent exciton-exciton interaction and energy relaxation under near-resonant circularly polarized ps pulsed excitation in single, multiple, or double coupled GaAs/AlGaAs quantum wells. Transient exciton spin splitting and relaxation were determined from time-resolved photoluminescence (TRPL) spectroscopy and polarimetry with a streak camera system. In contrast to standard TRPL measurements based on up-conversion and pump-probe techniques, the streak-camera setup allows for speedy spectroscopy and Stokes polarimetry measurements as a function of the exciton density and magnetic/electric field under near -resonant excitation (˜3 to 10 meV from the exciton resonance). For 6-nm and 14-nm GaAs/AlGaAs quantum wells at intermediate density (a few 10^10 cm-2), a spin splitting of 2 and 1 meV appeared instantly within 10 ps after excitation and exhibited a decay time constant of ˜100 and 500 ps, respectively. In the presence of magnetic fields, the spin splitting and relaxation dynamics became non-exponential and exhibited asymmetric and nonlinear dependence on the direction and magnitude of the field up to 10 Tesla. We analyzed the spin splitting and relaxation dynamics in terms of inter-exciton and intra-exciton exchange interaction and exciton-carrier interaction.
Transient electrically detected magnetic resonance spectroscopy applied to organic solar cells
Kraffert, Felix; Steyrleuthner, Robert; Meier, Christoph; Bittl, Robert; Behrends, Jan
2015-07-27
The influence of light-induced paramagnetic states on the photocurrent generated by polymer:fullerene solar cells is studied using spin-sensitive techniques in combination with laser-flash excitation. For this purpose, we developed a setup that allows for simultaneous detection of transient electron paramagnetic resonance as well as transient electrically detected magnetic resonance (trEDMR) signals from fully processed and encapsulated solar cells. Combining both techniques provides a direct link between photoinduced triplet excitons, charge transfer states, and free charge carriers as well as their influence on the photocurrent generated by organic photovoltaic devices. Our results obtained from solar cells based on poly(3-hexylthiophene) as electron donor and a fullerene-based electron acceptor show that the resonant signals observed in low-temperature (T = 80 K) trEDMR spectra can be attributed to positive polarons in the polymer as well as negative polarons in the fullerene phase, indicating that both centers are involved in spin-dependent processes that directly influence the photocurrent.
Low-Energy Excitation Spectra in the Excitonic Phase of Cobalt Oxides
NASA Astrophysics Data System (ADS)
Yamaguchi, Tomoki; Sugimoto, Koudai; Ohta, Yukinori
2017-04-01
We study the excitonic phase and low-energy excitation spectra of perovskite cobalt oxides. Constructing the five-orbital Hubbard model defined on the three-dimensional cubic lattice for the 3d bands of Pr0.5Ca0.5CoO3, we calculate the excitonic susceptibility in the normal state in the random-phase approximation (RPA) to show the presence of the instability toward excitonic condensation. On the basis of the excitonic ground state with a magnetic multipole obtained in the mean-field approximation, we calculate the dynamical susceptibility of the excitonic phase in the RPA and find that there appear a gapless collective excitation in the spin-transverse mode (Goldstone mode) and a gapful collective excitation in the spin-longitudinal mode (Higgs mode). The experimental relevance of our results is discussed.
Giant permanent dipole moment of two-dimensional excitons bound to a single stacking fault
NASA Astrophysics Data System (ADS)
Karin, Todd; Linpeng, Xiayu; Glazov, M. M.; Durnev, M. V.; Ivchenko, E. L.; Harvey, Sarah; Rai, Ashish K.; Ludwig, Arne; Wieck, Andreas D.; Fu, Kai-Mei C.
2016-07-01
We investigate the magneto-optical properties of excitons bound to single stacking faults in high-purity GaAs. We find that the two-dimensional stacking fault potential binds an exciton composed of an electron and a heavy hole, and we confirm a vanishing in-plane hole g -factor, consistent with the atomic-scale symmetry of the system. The unprecedented homogeneity of the stacking-fault potential leads to ultranarrow photoluminescence emission lines (with a full width at half-maximum ≲80 μ eV ) and reveals a large magnetic nonreciprocity effect that originates from the magneto-Stark effect for mobile excitons. These measurements unambiguously determine the direction and magnitude of the giant electric dipole moment (≳e ×10 nm ) of the stacking-fault exciton, making stacking faults a promising new platform to study interacting excitonic gases.
Tunable potentials and decoherence effect on polaron in nanostructures
NASA Astrophysics Data System (ADS)
Fotue, A. J.; Fobasso, M. F. C.; Kenfack, S. C.; Tiotsop, M.; Djomou, J.-R. D.; Ekosso, C. M.; Nguimeya, G.-P.; Danga, J. E.; Keumo Tsiaze, R. M.; Fai, L. C.
2016-06-01
We studied the effect of the tunable potential and decoherence of polaron in nanostructures. We have arbitrarily chosen eight potentials: the elliptical potential, square potential, triangular potential, the quadratic potential, the delta potential, the Gaussian potential, the pseudo-harmonic potential and Coulombic potential. In order to evaluate different polaronic parameters, we used the unitary transformation of LLP and the Pekar-type variational method (PTVM). This system can be considered as a two-level quantum system. We demonstrate in this work that the elliptical potential best confines the polaron and provides interesting information transfer, whereas, Gaussian, pseudo-harmonic and Coulombic potentials transfer information slowly. It is also found in this work that the Coulomb potential seems to be the most chaotic compared to the seven other used. This work confirms that the choice of a potential is crucial for the study of decoherence in nanostructures.
Use of site symmetry in supercell models of defective crystals: polarons in CeO2.
Evarestov, R A; Gryaznov, D; Arrigoni, M; Kotomin, E A; Chesnokov, A; Maier, J
2017-03-22
In supercell calculations of defective crystals, it is common to place a point defect or vacancy in the atomic position with the highest possible point symmetry. Then, the initial atomic structure is often arbitrary distorted before its optimization, which searches for the total energy minimum. In this paper, we suggest an alternative approach to the application of supercell models and show that it is necessary to preliminarily analyze the site symmetry of the split Wyckoff positions of the perfect crystal supercell atoms (which will be substituted or removed in defective crystals) and then perform supercell calculations with point defects for different possible site symmetries, to find the energetically most favorable defect configuration, which does not necessarily correspond to the highest site symmetry. Using CeO2 as an example, it is demonstrated that this use of the site symmetry of the removed oxygen atoms in the supercells with vacancies allows us to obtain all the possible atomic and magnetic polaron configurations, and predict which vacancy positions correspond to the lowest formation energies associated with small polarons. We give a simple symmetry based explanation for the existence of controversies in the literature on the nature of the oxygen vacancies in CeO2. In particular, the experimentally observed small polaron formation could arise for oxygen vacancies with the lowest Cs site symmetry, which exist in 3 × 3 × 3 and larger supercells. The results of first principles calculations using a linear combination of atomic orbitals and hybrid exchange-correlation functionals are compared with those from previous studies, obtained using a widely used DFT+U approach.
Polaron effects in asymmetric semiconductor quantum-well structures
NASA Astrophysics Data System (ADS)
Shi, Jun-Jie; Zhu, Xiu-Qin; Liu, Zi-Xin; Pan, Shao-Hua; Li, Xing-Yi
1997-02-01
In this paper, polaron effects in asymmetric quantum-well structures (QW's) are investigated by using second-order perturbation theory and the modified Lee-Low-Pines (LLP) variational method. By applying the Green"s-function method, explicit analytical expressions for the electron extended-state wave functions and the density of states in a general step QW's are given. Within the framework of second-order perturbation theory, the ground-state polaron binding energy and effective mass in step and asymmetric single QW"s are studied as due to the interface optical phonons, confined bulklike LO and half-space LO phonons. The full energy spectrum is included in our calculations. The effects of the finite electronic confinement potential and the subband nonparabolicity are also considered. The relative importance of the different phonon modes is analyzed. By means of the modified LLP variational method, the binding energy of a polaron confined to asymmetric single QW's is also investigated. Our results show that in ordinary asymmetric QW"s, the asymmetry of the QW's has a significant influence on the polaron effect, which has a close relationship to the interface phonon dispersion. When the well width and one side barrier height of asymmetric single QW"s are fixed and identical with those of symmetric QW's, the polaron binding energy in asymmetric QW"s is always smaller than that in symmetric QW's. We have also found that it is necessary to include the continuum energy spectrum as intermediate states in the perturbation calculations in order to obtain the correct results; the subband nonparabolicity has a small influence on the polaron effect. Comparing our results obtained by using two different methods, good agreement is found.
Numerical simulation of photoexcited polaron states in water
Zemlyanaya, E. V. Volokhova, A. V.; Amirkhanov, I. V.; Puzynin, I. V.; Puzynina, T. P.; Rikhvitskiy, V. S.; Lakhno, V. D.; Atanasova, P. Kh.
2015-10-28
We consider the dynamic polaron model of the hydrated electron state on the basis of a system of three nonlinear partial differential equations with appropriate initial and boundary conditions. A parallel numerical algorithm for the numerical solution of this system has been developed. Its effectiveness has been tested on a few multi-processor systems. A numerical simulation of the polaron states formation in water under the action of the ultraviolet range laser irradiation has been performed. The numerical results are shown to be in a reasonable agreement with experimental data and theoretical predictions.
Exciton dispersion in molecular solids.
Cudazzo, Pierluigi; Sottile, Francesco; Rubio, Angel; Gatti, Matteo
2015-03-25
The investigation of the exciton dispersion (i.e. the exciton energy dependence as a function of the momentum carried by the electron-hole pair) is a powerful approach to identify the exciton character, ranging from the strongly localised Frenkel to the delocalised Wannier-Mott limiting cases. We illustrate this possibility at the example of four prototypical molecular solids (picene, pentacene, tetracene and coronene) on the basis of the parameter-free solution of the many-body Bethe-Salpeter equation. We discuss the mixing between Frenkel and charge-transfer excitons and the origin of their Davydov splitting in the framework of many-body perturbation theory and establish a link with model approaches based on molecular states. Finally, we show how the interplay between the electronic band dispersion and the exchange electron-hole interaction plays a fundamental role in setting the nature of the exciton. This analysis has a general validity holding also for other systems in which the electron wavefunctions are strongly localized, as in strongly correlated insulators.
Exciton dispersion in molecular solids
NASA Astrophysics Data System (ADS)
Cudazzo, Pierluigi; Sottile, Francesco; Rubio, Angel; Gatti, Matteo
2015-03-01
The investigation of the exciton dispersion (i.e. the exciton energy dependence as a function of the momentum carried by the electron-hole pair) is a powerful approach to identify the exciton character, ranging from the strongly localised Frenkel to the delocalised Wannier-Mott limiting cases. We illustrate this possibility at the example of four prototypical molecular solids (picene, pentacene, tetracene and coronene) on the basis of the parameter-free solution of the many-body Bethe-Salpeter equation. We discuss the mixing between Frenkel and charge-transfer excitons and the origin of their Davydov splitting in the framework of many-body perturbation theory and establish a link with model approaches based on molecular states. Finally, we show how the interplay between the electronic band dispersion and the exchange electron-hole interaction plays a fundamental role in setting the nature of the exciton. This analysis has a general validity holding also for other systems in which the electron wavefunctions are strongly localized, as in strongly correlated insulators.
Superexchange coupling and electron transfer in globular proteins via polaron excitations.
Chuev, G N; Lakhno, V D; Ustitnin, M N
2000-06-01
The polaron approach is used to treat long-range electron transfersbetween globular proteins. A rate expression for the polaron transfer model is given along with a description of appropriate conditions forits use. Assuming that electrons transfer via a superexchange couplingdue to a polaron excitation, we have estimated the distance dependenceof the rate constant for the self-exchange reactions between globularproteins in solutions. The distance dependence of the polaron coupling andsolvent reorganization energy are provided as a basis forunderstanding and interpreting a long-range electron transfer experiment.The difficulties and problems of the polaron treatment of long-rangeelectron transfers are discussed, and suggestions for new experimentsare made.
Excitonic polaritons in Fibonacci quasicrystals.
Hendrickson, J; Richards, B C; Sweet, J; Khitrova, G; Poddubny, A N; Ivchenko, E L; Wegener, M; Gibbs, H M
2008-09-29
The fabrication and characterization of light-emitting one-dimensional photonic quasicrystals based on excitonic resonances is reported. The structures consist of high-quality GaAs/AlGaAs quantum wells grown by molecular-beam epitaxy with wavelength-scale spacings satisfying a Fibonacci sequence. The polaritonic (resonant light-matter coupling) effects and light emission originate from the quantum well excitonic resonances. Measured reflectivity spectra as a function of detuning between emission and Bragg wavelength are in good agreement with excitonic polariton theory. Photoluminescence experiments show that active photonic quasicrystals, unlike photonic crystals, can be good light emitters: While their long-range order results in a stopband similar to that of photonic crystals, the lack of periodicity results in strong emission.
NASA Astrophysics Data System (ADS)
Bastardis, Roland; Guihéry, Nathalie; de Graaf, Coen
2006-07-01
The low-energy spectrum of the Zener polaron in half-doped manganite is studied by means of correlated ab initio calculations. It is shown that the electronic structure of the low-energy states results from a subtle interplay between double-exchange configurations and O 2pσ to Mn 3d charge-transfer configurations that obey a Heisenberg logic. The comparison of the calculated spectrum to those predicted by the Zener Hamiltonian reveals that this simple description does not correctly reproduces the Zener polaron physics. A better reproduction of the calculated spectrum is obtained with either a Heisenberg model that considers a purely magnetic oxygen or the Girerd-Papaefthymiou double-exchange model. An additional significant improvement is obtained when different antiferromagnetic contributions are combined with the double-exchange model, showing that the Zener polaron spectrum is actually ruled by a refined double-exchange mechanism where non-Hund atomic states play a non-negligible role. Finally, eight states of a different nature have been found to be intercalated in the double-exchange spectrum. These states exhibit an O to Mn charge transfer, implying a second O 2p orbital of approximate π character instead of the usual σ symmetry. A small mixing of the two families of states occurs, accounting for the final ordering of the states.
The strong-coupling polaron in reduced dimensionality
NASA Astrophysics Data System (ADS)
Sahoo, Satyabrata
1998-03-01
Based on the LLP-H approach, a detailed study of the electron confinement in a polar semiconductor heterostructure has been made to derive analytically the ground state energy and the effective mass of the Fröhlich polaron in quasi-two-dimensional (Q2D) and quasi-one-dimensional (Q1D) systems.
Polaron mass of charge carriers in semiconductor quantum wells
Maslov, A. Yu. Proshina, O. V.
2015-10-15
A theory of the interaction of charge carriers with optical phonons in a quantum well is developed with consideration for interface optical phonons. The dependence of the polaron effective mass on the quantum-well dimensions and dielectric characteristics of barriers is analyzed in detail. It is shown that, in narrow quantum wells, a quasi-two-dimensional polaron can be formed. In this case, however, the interaction parameters are defined by the charge-carrier effective mass in the quantum well and by the frequencies of interface optical phonons. If barriers are made of a nonpolar material, the polaron effective mass depends on the quantum-well width. As the quantum-well width is increased, a new mechanism of enhancement of the electron–phonon interaction develops. The mechanism is implemented, if the optical phonon energy is equal to the energy of one of the electronic transitions. This condition yields an unsteady dependence of the polaron effective mass on the quantum-well width.
A Nonempirical Comparison of the Polaron and Mowat Sensor.
ERIC Educational Resources Information Center
Moore, Karyl A.
1995-01-01
This article compares two electronic aids that send out an elliptical cone of ultrasonic sound that bounces back as a usable information signal for individuals with blindness. The Polaron is better for people who are predominantly route travelers or with limited hand use. The Mowat Sensor is better for travelers in a variety of environments. (JDD)
Exciton-photon correlations in bosonic condensates of exciton-polaritons
Kavokin, Alexey V.; Sheremet, Alexandra S.; Shelykh, Ivan A.; Lagoudakis, Pavlos G.; Rubo, Yuri G.
2015-01-01
Exciton-polaritons are mixed light-matter quasiparticles. We have developed a statistical model describing stochastic exciton-photon transitions within a condensate of exciton polaritons. We show that the exciton-photon correlator depends on the rate of incoherent exciton-photon transformations in the condensate. We discuss implications of this effect for the quantum statistics of photons emitted by polariton lasers. PMID:26153979
Vinolin, Ada; Peter, A. John
2015-06-24
Magneto-LO-polaron in a cylindrical GaAs{sub 0.9} P{sub 0.1} / GaAs{sub 0.6} P{sub 0.4} quantum dot is investigated taking into consideration of geometrical confinement effect. The effects of phonon on the exciton binding energy and the interband emission energy as a function of dot radius are found. The calculations are performed within the single band effective mass approximation using the variational method based on the Lee-Low-Pine LLP transformation.
Optical transition energy of magneto-polaron in a GaAs0.9P0.1/GaAs0.6P0.4 quantum dot
NASA Astrophysics Data System (ADS)
Vinolin, Ada; Peter, A. John
2015-06-01
Magneto-LO-polaron in a cylindrical GaAs0.9 P0.1 / GaAs0.6 P0.4 quantum dot is investigated taking into consideration of geometrical confinement effect. The effects of phonon on the exciton binding energy and the interband emission energy as a function of dot radius are found. The calculations are performed within the single band effective mass approximation using the variational method based on the Lee-Low-Pine LLP transformation.
NASA Astrophysics Data System (ADS)
Matsunaga, Ryusuke; Matsuda, Kazunari; Kanemitsu, Yoshihiko
2009-03-01
We have performed micro-photoluminescence (PL) spectroscopy for single carbon nanotubes under magnetic fields at various temperatures. Sharp PL spectra of single carbon nanotubes allow us to directly observe the dark exciton PL peak a few meV below the bright exciton PL peak due to the Aharonov-Bohm effect [1]. From the PL intensity ratio of the dark to the bright excitons under magnetic fields, we found that the non-equilibrium (non-Boltzmann) distribution occurs between the bright and dark states, because phonons cannot scatter excitons between the two states with different parities [2]. Furthermore, we discuss the diameter dependence of the exciton population of the bright and dark states in single carbon nanotubes. [1] R. Matsunaga, K. Matsuda, and Y. Kanemitsu, Phys. Rev. Lett. 101, 147404 (2008). [2] V. Perebeinos, J. Tersoff, and Ph. Avouris, Nano Lett. 5, 2495 (2005).
The structure of nanoscale polaron correlations in the layered manganites
NASA Astrophysics Data System (ADS)
Campbell, Branton
2002-03-01
Recent x-ray and neutron scattering experiments have uncovered nanoscale polaron correlations that play an essential role in the colossal magnetoresistive (CMR) behavior of the perovskite manganites. Short-range polaronic order decreases the charge-carrier mobility of the high-temperature paramagnetic state, and subsequently becomes unstable at the ferromagnetic transition, contributing to a pronounced resistivity decrease at T_C. In the bilayered perovskite system La_2-2xSr_1+2xMn_2O7 (0.3 < x < 0.5), weak x-ray diffuse scattering maxima reveal a one-dimensional incommensurate structural modulation with wavevector q = (0.3, 0, ± 1) and a correlation length of 10 to 30 Angstroms. A crystallographic analysis of the diffuse satellite intensities yields a longitudinal Jahn-Teller stretch mode suggestive of charge-density-wave fluctuations. Within the correlated regions, polaronic eg electrons form a striped pattern of occupied d(3x^2-r^2) orbitals. Dynamic polaron correlations of the zig-zag orbital type are also observed above TC and exhibit distinctly glassy behavior. These structures provide unique insights into the nature of strongly correlated polaronic systems. Collaborators: R. Osborn, D.N. Argyriou, S. Rosenkranz, L. Vasiliu-Doloc, J.F. Mitchell, S.K. Sinha, J.W. Lynn, C.D. Ling, Z. Islam, U. Ruett, and A. Berger. This work was supported by the U.S. DOE Office of Science contract No. W-31-109-ENG-38.
Measurement of exciton correlations using electrostatic lattices
NASA Astrophysics Data System (ADS)
Remeika, M.; Leonard, J. R.; Dorow, C. J.; Fogler, M. M.; Butov, L. V.; Hanson, M.; Gossard, A. C.
2015-09-01
We present a method for determining correlations in a gas of indirect excitons in a semiconductor quantum well structure. The method involves subjecting the excitons to a periodic electrostatic potential that causes modulations of the exciton density and photoluminescence (PL). Experimentally measured amplitudes of energy and intensity modulations of exciton PL serve as an input to a theoretical estimate of the exciton correlation parameter and temperature. We also present a proof-of-principle demonstration of the method for determining the correlation parameter and discuss how its accuracy can be improved.
Exciton size and quantum transport in nanoplatelets.
Pelzer, Kenley M; Darling, Seth B; Gray, Stephen K; Schaller, Richard D
2015-12-14
Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.
Exciton size and quantum transport in nanoplatelets
NASA Astrophysics Data System (ADS)
Pelzer, Kenley M.; Darling, Seth B.; Gray, Stephen K.; Schaller, Richard D.
2015-12-01
Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.
Exciton size and quantum transport in nanoplatelets
Pelzer, Kenley M. Gray, Stephen K.; Darling, Seth B.; Schaller, Richard D.
2015-12-14
Two-dimensional nanoplatelets (NPLs) are an exciting class of materials with promising optical and energy transport properties. The possibility of efficient energy transport between nanoplatelets raises questions regarding the nature of energy transfer in these thin, laterally extended systems. A challenge in understanding exciton transport is the uncertainty regarding the size of the exciton. Depending on the material and defects in the nanoplatelet, an exciton could plausibly extend over an entire plate or localize to a small region. The variation in possible exciton sizes raises the question how exciton size impacts the efficiency of transport between nanoplatelet structures. Here, we explore this issue using a quantum master equation approach. This method goes beyond the assumptions of Förster theory to allow for quantum mechanical effects that could increase energy transfer efficiency. The model is extremely flexible in describing different systems, allowing us to test the effect of varying the spatial extent of the exciton. We first discuss qualitative aspects of the relationship between exciton size and transport and then conduct simulations of exciton transport between NPLs for a range of exciton sizes and environmental conditions. Our results reveal that exciton size has a strong effect on energy transfer efficiency and suggest that manipulation of exciton size may be useful in designing NPLs for energy transport.
Fine structure of a resonantly excited p -shell exciton in a CdTe quantum dot
NASA Astrophysics Data System (ADS)
Smoleński, T.; Kazimierczuk, T.; Goryca, M.; Wojnar, P.; Kossacki, P.
2016-05-01
We present a polarization-resolved photoluminescence excitation study of the absorption spectrum of a p -shell neutral exciton in a single CdTe/ZnTe quantum dot. We find that the fine structure of the p -shell exciton is completely analogous to the fine structure of the s -shell exciton, including the selection rules and the effects of a magnetic field applied in Faraday and Voigt configurations. The energy spectrum of the p -shell exciton is found to be well described by introducing respective isotropic and anisotropic constants of the exchange interaction between a p -shell electron and a p -shell hole. The typical values of these exchange constants averaged over several randomly selected quantum dots yield δ0p p=(0.92 ±0.16 ) meV and δ1p p=(0.58 ±0.25 ) meV. Additionally, we demonstrate that the nonresonant relaxation of the p -shell exciton conserves the exciton spin to a very high degree for both bright and dark exciton configurations.
Exciton-exciton scattering: Composite boson versus elementary boson
NASA Astrophysics Data System (ADS)
Combescot, M.; Betbeder-Matibet, O.; Combescot, R.
2007-05-01
This paper shows the necessity of introducing a quantum object, the “coboson,” to properly describe, through a fermion scheme, any composite particle, such as the exciton, which is made of two fermions. Although commonly dealt with as elementary bosons, these composite bosons—cobosons in short—differ from them due to their composite nature which makes the handling of their many-body effects quite different from the existing treatments valid for elementary bosons. As a direct consequence of this composite nature, there is no correct way to describe the interaction between cobosons as a potential V . This is rather dramatic because, with the Hamiltonian not written as H=H0+V , all the usual approaches to many-body effects fail. In particular, the standard form of the Fermi golden rule, written in terms of V , cannot be used to obtain the transition rates of two cobosons. To get them, we have had to construct an unconventional expression for this Fermi golden rule in which H only appears. Making use of this expression, we give here a detailed calculation of the time evolution of two excitons. We compare the results of this exact approach with the ones obtained by using an effective bosonic Hamiltonian in which the excitons are considered as elementary bosons with effective scatterings between them, these scatterings resulting from an elaborate mapping between the two-fermion space and the ideal boson space. We show that the relation between the inverse lifetime and the sum of the transition rates for elementary bosons differs from the one of the composite bosons by a factor of 1/2 , so that it is impossible to find effective scatterings between bosonic excitons giving these two physical quantities correctly, whatever the mapping from composite bosons to elementary bosons is. The present paper thus constitutes a strong mathematical proof that, in spite of a widely spread belief, we cannot forget the composite nature of these cobosons, even in the extremely low
Spatially indirect excitons in coupled quantum wells
Lai, Chih-Wei Eddy
2004-03-01
Microscopic quantum phenomena such as interference or phase coherence between different quantum states are rarely manifest in macroscopic systems due to a lack of significant correlation between different states. An exciton system is one candidate for observation of possible quantum collective effects. In the dilute limit, excitons in semiconductors behave as bosons and are expected to undergo Bose-Einstein condensation (BEC) at a temperature several orders of magnitude higher than for atomic BEC because of their light mass. Furthermore, well-developed modern semiconductor technologies offer flexible manipulations of an exciton system. Realization of BEC in solid-state systems can thus provide new opportunities for macroscopic quantum coherence research. In semiconductor coupled quantum wells (CQW) under across-well static electric field, excitons exist as separately confined electron-hole pairs. These spatially indirect excitons exhibit a radiative recombination time much longer than their thermal relaxation time a unique feature in direct band gap semiconductor based structures. Their mutual repulsive dipole interaction further stabilizes the exciton system at low temperature and screens in-plane disorder more effectively. All these features make indirect excitons in CQW a promising system to search for quantum collective effects. Properties of indirect excitons in CQW have been analyzed and investigated extensively. The experimental results based on time-integrated or time-resolved spatially-resolved photoluminescence (PL) spectroscopy and imaging are reported in two categories. (i) Generic indirect exciton systems: general properties of indirect excitons such as the dependence of exciton energy and lifetime on electric fields and densities were examined. (ii) Quasi-two-dimensional confined exciton systems: highly statistically degenerate exciton systems containing more than tens of thousands of excitons within areas as small as (10 micrometer)^{2} were
NASA Astrophysics Data System (ADS)
Basel, Tek Prasad
We studied optical, electrical, and magnetic field responses of films and devices based on organic semiconductors that are used for organic light emitting diodes (OLEDs) and photovoltaic (OPV) solar cell applications. Our studies show that the hyperfine interaction (HFI)-mediated spin mixing is the key process underlying various magnetic field effects (MFE) and spin transport in aluminum tris(8-hydroxyquinoline)[Alq3]-based OLEDs and organic spin-valve (OSV). Conductivity-detected magnetic resonance in OLEDs and magneto-resistance (MR) in OSVs show substantial isotope dependence. In contrast, isotope-insensitive behavior in the magneto-conductance (MC) of same devices is explained by the collision of spin ½ carriers with triplet polaron pairs. We used steady state optical spectroscopy for studying the energy transfer dynamics in films and OLEDs based on host-guest blends of the fluorescent polymer and phosphorescent molecule. We have also studied the magnetic-field controlled color manipulation in these devices, which provide a strong proof for the `polaron-pair' mechanism underlying the MFE in organic devices. The critical issue that hampers organic spintronics device applications is significant magneto-electroluminescence (MEL) at room temperature (RT). Whereas inorganic spin valves (ISVs) show RT magneto-resistance, MR>80%, however, the devices do not exhibit electroluminescence (EL). In contrast, OLEDs show substantive EL emission, and are particularly attractive because of their flexibility, low cost, and potential for multicolor display. We report a conceptual novel hybrid organic/inorganic spintronics device (h-OLED), where we employ both ISV with large MR at RT, and OLED that has efficient EL emission. We investigated the charge transfer process in an OPV solar cell through optical, electrical, and magnetic field measurements of thin films and devices based on a low bandgap polymer, PTB7 (fluorinated poly-thienothiophene-benzodithiophene). We found that
Contrastive analysis of multiple exciton generation theories
NASA Astrophysics Data System (ADS)
Tan, Hengyu; Chang, Qing
2015-10-01
Multiple exciton generation (MEG) is an effect that semiconductor nanocrystals (NCs) quantum dots (QDs) generate multiple excitons (electron-hole pairs) through absorbing a single high energy photon. It can translate the excess photon energy of bandgap (Eg) into new excitons instead of heat loss and improve the photovoltaic performance of solar cells. However, the theories of MEG are not uniform. The main MEG theories can be divided into three types. The first is impact ionization. It explains MEG through a conventional way that a photogenerated exciton becomes multiple excitons by Coulomb interactions between carriers. The Second is coherent superposition of excitonic states. Multiple excitons are generated by the coherent superposition of single photogenerated exciton state with enough excess momentum and the two-exciton state with the same momentum. The third is excitation via virtual excitonic states. The nanocrystals vacuum generates a virtual biexciton by coulomb coupling between two valence band electrons. The virtual biexciton absorbing a photon with an intraband optical transition is converted into a real biexciton. This paper describes the MEG influence on solar photoelectric conversion efficiency, concludes and analyzes the fundamentals of different MEG theories, the MEG experimental measure, their merits and demerits, calculation methods of generation efficiency.
Coherent Exciton Dynamics in Atomically Thin Semiconductors
NASA Astrophysics Data System (ADS)
Li, Xiaoqin (Elaine)
The near band-edge optical response of an emerging class of semiconductors, known as the transitional metal dichalcogenides (TMDs), is dominated by tightly-bound excitons and charged excitons (i.e. trions). A fundamental property of these quasiparticles (excitons and trions) is quantum decoherence time, which reflects irreversible quantum dissipation arising from system (excitons and trions) and bath (vacuum and other quasiparticles) interactions and determines the timescale during which excitons can be coherently manipulated. Dephasing time is also equivalent to the intrinsic homogeneous linewidth of exciton resonance. In addition, excitons in TMDs are localized at the corners of the Brillouin zone and provide a convenient way to optical manipulate the valley degree of freedom, which may act as a useful information carrier analogous to electronic charge or spin. Direct measurement of valley coherence time is challenging because it corresponds to a non-radiative coherence between two degenerate states. Using ultrafast multi-dimensional optical spectroscopy, we investigate the intrinsic homogeneous linewidth of excitons, exciton valley coherence as well as coupling between excitons and trions. Our studies reveal coherent electronic dynamics on the order of ~100 fs in monolayer TMDs. We gratefully acknowledge financial support from NSF, AFOSR, and the Welch Foundation.
NASA Astrophysics Data System (ADS)
Meier, Christoph; Teutloff, Christian; Behrends, Jan; Bittl, Robert; Astakhov, Oleksandr; Lips, Klaus
2016-07-01
Electrically detected magnetic resonance (EDMR) spectroscopy is employed to study the influence of triplet excitons on the photocurrent in state-of-the-art microcrystalline silicon thin-film solar cells. These triplet excitons are used as sensitive spin probes for the investigation of their electronic and nuclear environment in this mixed-phase material. According to low-temperature EDMR results obtained from solar cells with different
A polaron model for electron transfer in globular proteins.
Chuev, G N; Lakhno, V D
1993-07-07
Polaron models have been considered for the electron states in protein globules existing in a solvent. These models account for two fundamental effects, viz, polarization interaction of an electron with the conformational vibrations and the heterogeneity of the medium. Equations have been derived to determine the electron state in a protein globule. The parameters of this state show that it is an extended state with an energy of 2 eV. The electron transfer rate for cyt C self-exchange reaction has been calculated in the polaron model. Reorganization energy, tunneling matrix element and the rate constant have also been estimated. The results are compared with experimental data. The influence of model parameters on the significance of the data obtained has been studied. The potentialities of the model are discussed.
Polaron theory of electrons solvated in molten salts
NASA Astrophysics Data System (ADS)
Malescio, G.; Parrinello, M.
1987-01-01
A suitably modified version of the polaron theory of Chandler et al. [J. Chem. Phys. 81, 1975 (1984)] is applied to the study of the solvation of electrons in molten salts. The results obtained compare favorably with recent numerical simulations and confirm the picture of the formation in the melt of an F-center analog. A novel expression for the explicit evaluation of the electron kinetic energy is given.
The effective excitonic g factors of Mn-doped InAs nanowires
NASA Astrophysics Data System (ADS)
Xiong, Wen
2017-04-01
Based on the derived eight-band k · p Hamiltonian, the electronic structures of Mn-doped InAs nanowires in the magnetic field are calculated. We find the lowest optical transition will be split to four individual transitions when the magnetic field is applied along z axis, and two of them are σ polarized light. Furthermore, the Zeeman splitting energy at the Γ point of two σ polarized light will increase nonlinearly as the increase of the magnetic field. Additionally, an effective excitonic g factor at the Γ point is defined, and the effective excitonic g factors will decrease greatly with the increase of the radius of nanowires and the decrease of the concentration of manganese ions, while the effective excitonic g factors decrease slightly when the magnetic field increases. Interestingly, the effective excitonic g factors can experience a substantial decrease when the temperature increases from 10 K to 100 K and is almost not affected when the temperature varies from 100 K to 300 K. Therefore, we can infer that large effective excitonic g factors can be obtained when small radius of nanowires, high concentration of manganese ions and low temperature are satisfied.
Rotational polarons and transport in short molecular devices
NASA Astrophysics Data System (ADS)
Ulloa, Sergio E.; Sierra-Ortega, J.; Zhang, Wei
2003-03-01
In many organic materials and/or complex molecular structures, there are twist/rotational modes that appear at low temperature and are easily excitable. The interaction between these rotational phonon modes and electrons generates a new quasiparticle, the rotational polaron. We study here a two-site rotational Holstein polaron. Our model gives nontrivial polaron physics due to anharmonic oscillations and nonlinear electron-phonon interactions. The results are relevant for molecular electronic devices composed of two molecular units with excitable intra-molecular rotations. Analytical and numerical calculations allow a full quantum mechanical description. We study all frequency and coupling regimes, paying special attention to the transition/crossover between different coupling ratios. We find that under resonant conditions between the electron level splitting and the phonon frequency, complex level crossings and anticrossings occur, indicating mixing of excited states with different characters, which depend on underlying symmetries of the system. The mixing is accompanied by charge and phonon amplitude transfer which yields observable signatures in electronic transport through this system. Supported by NSF-NIRT, US-DOE, and OU-CMSS.
Unravelling Small-Polaron Transport in Metal Oxide Photoelectrodes.
Rettie, Alexander J E; Chemelewski, William D; Emin, David; Mullins, C Buddie
2016-02-04
Transition-metal oxides are a promising class of semiconductors for the oxidation of water, a process that underpins both photoelectrochemical water splitting and carbon dioxide reduction. However, these materials are limited by very slow charge transport. This is because, unlike conventional semiconductors, material aspects of metal oxides favor the formation of slow-moving, self-trapped charge carriers: small polarons. In this Perspective, we seek to highlight the salient features of small-polaron transport in metal oxides, offer guidelines for their experimental characterization, and examine recent transport studies of two prototypical oxide photoanodes: tungsten-doped monoclinic bismuth vanadate (W:BiVO4) and titanium-doped hematite (Ti:α-Fe2O3). Analysis shows that conduction in both materials is well-described by the adiabatic small-polaron model, with electron drift mobility (distinct from the Hall mobility) values on the order of 10(-4) and 10(-2) cm(2) V(-1) s(-1), respectively. Future directions to build a full picture of charge transport in this family of materials are discussed.
Hole polaron formation and migration in olivine phosphate materials
NASA Astrophysics Data System (ADS)
Johannes, M. D.; Hoang, Khang; Allen, J. L.; Gaskell, K.
2012-03-01
By combining first-principles calculations and experimental x-ray photoemission (XPS) spectroscopy measurements, we investigate the electronic structure of potential Li-ion battery cathode materials LiMPO4 (M=Mn, Fe, Co, Ni) to uncover the underlying mechanisms that determine small hole polaron formation and migration. We show that small hole polaron formation depends on features in the electronic structure near the valence-band maximum and that, calculationally, these features depend on the methodology chosen for dealing with the correlated nature of the transition-metal d-derived states in these systems. Comparison with experiment reveals that a hybrid functional approach is superior to GGA+U in correctly reproducing the XPS spectra. Using this approach, we find that LiNiPO4 cannot support small hole polarons, but that the other three compounds can. The migration barrier is determined mainly by the strong- or weak-bonding nature of the states at the top of the valence band, resulting in a substantially higher barrier for LiMnPO4 than for LiCoPO4 or LiFePO4.
Novel, discontinuous polaron transition in a two-band model
NASA Astrophysics Data System (ADS)
Moeller, Mirko M.; Sawatzky, George A.; Berciu, Mona
The coupling of charge carriers (electrons or holes) to phonons leads to the formation of a polaron, a coherent quasi-particle consisting of the charge carrier and the cloud of phonons surrounding it and moving coherently with it. Here we present exact diagonalization and momentum average approximation results for the single polaron properties of a two-band model with phonon modulated hopping, inspired by the perovskite BaBiO3. For large coupling we find that the ground state momentum changes discontinuously from k = π to k = 0 . Such sharp transitions of the polaron's ground state properties cannot occur in the well-studied models of the Holstein or Fröhlich type in which the carrier-phonon coupling modulates the on-site energies. However, they can occur in models where the carrier-phonon coupling modulates the hopping integrals such as the SSH model for which a similar yet smooth transition of the ground state momentum was recently shown to exist. We compare our findings to the SSH model and point out qualitative differences which we believe to be due to the two band nature of our model versus the single band SSH model. This work was supported by NSERC, QMI and the UBC 4YF.
Lloyd-Hughes, J. Failla, M.; Ye, J.; Jones, S. P. P.; Teo, K. L.; Jagadish, C.
2015-05-18
The cyclotron resonance of polarons in Zn{sub 1−x}Mg{sub x}O/ZnO heterostructures (with 0.15
Exciton-polariton integrated circuits
NASA Astrophysics Data System (ADS)
Liew, T. C. H.; Kavokin, A. V.; Ostatnický, T.; Kaliteevski, M.; Shelykh, I. A.; Abram, R. A.
2010-07-01
We show that logical signals encoded in bistable states in semiconductor microcavities can be generated and controlled electronically by exploiting the electrical sensitivity of Tamm-plasmon-exciton-polariton modes. The signals can be transported along polariton neurons, created with a patterned metal surface. Using the Gross-Pitaevskii equations, we simulate an electrically controlled transistor and find that high repetition rates (10 GHz) are possible.
Effect of interchain coupling on the excited polaron in conjugated polymers
NASA Astrophysics Data System (ADS)
Li, Xiao-xue; Chen, Gang
2017-02-01
Based on the one-dimensional extended Su-Schrieffer-Heeger model, we theoretically investigate the effect of interchain coupling on the formation and polarization of the single-excited state of polaron in conjugated polymers. It is found that there exists a turnover value of the coupling strength, over which the excited polaron could not be formed in either of the two coupled chains. Instead, a polaron-like particle is localized at the center of each chain. In addition, we also find that the reverse polarization of the excited polaron could be enhanced for some cases in polymer when the interchain coupling becomes strong until it exceeds the critical value.
Exciton Seebeck effect in molecular systems.
Yan, Yun-An; Cai, Shaohong
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.
Exciton Seebeck effect in molecular systems
Yan, Yun-An; Cai, Shaohong
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.
Control of Exciton Valley Coherence in Transition Metal Dichalcogenide Monolayers
NASA Astrophysics Data System (ADS)
Wang, G.; Marie, X.; Liu, B. L.; Amand, T.; Robert, C.; Cadiz, F.; Renucci, P.; Urbaszek, B.
2016-10-01
The direct gap interband transitions in transition metal dichalcogenide monolayers are governed by chiral optical selection rules. Determined by laser helicity, optical transitions in either the K+ or K- valley in momentum space are induced. Linearly polarized laser excitation prepares a coherent superposition of valley states. Here, we demonstrate the control of the exciton valley coherence in monolayer WSe2 by tuning the applied magnetic field perpendicular to the monolayer plane. We show rotation of this coherent superposition of valley states by angles as large as 30° in applied fields up to 9 T. This exciton valley coherence control on the ps time scale could be an important step towards complete control of qubits based on the valley degree of freedom.
Hu, Miao; Bi, Cheng; Yuan, Yongbo; Xiao, Zhengguo; Dong, Qingfeng; Shao, Yuchuan; Huang, Jinsong
2015-05-13
The nonexcitonic character for organometal trihalide perovskites is demonstrated by examining the field-dependent exciton dissociation behavior. It is found that photogenerated excitons can be effectively dissociated into free charges inside perovskite without the assistance of charge extraction layer or external field, which is a stark contrast to the charge-separation behavior in excitonic materials in the same photovoltaic operation system.
Hu, Miao; Bi, Cheng; Yuan, Yongbo; ...
2015-01-15
The nonexcitonic character for organometal trihalide perovskites is demonstrated by examining the field-dependent exciton dissociation behavior. Moreover, it is found that photogenerated excitons can be effectively dissociated into free charges inside perovskite without the assistance of charge extraction layer or external field, which is a stark contrast to the charge-separation behavior in excitonic materials in the same photovoltaic operation system.
Ground state energy of N Frenkel excitons
NASA Astrophysics Data System (ADS)
Pogosov, W.; Combescot, M.
2009-03-01
By using the composite many-body theory for Frenkel excitons we have recently developed, we here derive the ground state energy of N Frenkel excitons in the Born approximation through the Hamiltonian mean value in a state made of N identical Q = 0 excitons. While this quantity reads as a density expansion in the case of Wannier excitons, due to many-body effects induced by fermion exchanges between N composite particles, we show that the Hamiltonian mean value for N Frenkel excitons only contains a first order term in density, just as for elementary bosons. Such a simple result comes from a subtle balance, difficult to guess a priori, between fermion exchanges for two or more Frenkel excitons appearing in Coulomb term and the ones appearing in the N exciton normalization factor - the cancellation being exact within terms in 1/Ns where Ns is the number of atomic sites in the sample. This result could make us naively believe that, due to the tight binding approximation on which Frenkel excitons are based, these excitons are just bare elementary bosons while their composite nature definitely appears at various stages in the precise calculation of the Hamiltonian mean value.
Tang, Yanhao; Xie, Wei; McGuire, John A. Lai, Chih Wei; Mandal, Krishna C.
2015-09-21
We analyze exciton spin dynamics in GaSe under nonresonant circularly polarized optical pumping with an exciton spin-flip rate-equation model. The model reproduces polarized time-dependent photoluminescence measurements in which the initial circular polarization approaches unity even when pumping with 0.15 eV excess energy. At T = 10 K, the exciton spin relaxation exhibits a biexponential decay with sub-20 ps and >500 ps time constants, which are also reproduced by the rate-equation model assuming distinct spin-relaxation rates for hot (nonequilibrium) and cold band-edge excitons.
NASA Astrophysics Data System (ADS)
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) and a strong (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.
Josephson effects in condensates of excitons and exciton polaritons
Shelykh, I. A.; Solnyshkov, D. D.; Pavlovic, G.; Malpuech, G.
2008-07-15
We analyze theoretically the phenomena related to the Josephson effect for exciton and polariton condensates, taking into account their specific spin degrees of freedom. We distinguish between two types of Josephson effects: the extrinsic effect, related to the coherent tunneling of particles with the same spin between two spatially separated potential traps, and the intrinsic effect, related to the 'tunneling' between different spinor components of the condensate within the same trap. We show that the Josephson effect in the nonlinear regime can lead to nontrivial polarization dynamics and produce spontaneous separation of the condensates with opposite polarization in real space.
Relative Ordering between Bright and Dark Excitons in Single-walled Carbon Nanotubes
Zhou, Weihang; Nakamura, Daisuke; Liu, Huaping; Kataura, Hiromichi; Takeyama, Shojiro
2014-01-01
The ordering and relative energy splitting between bright and dark excitons are critical to the optical properties of single-walled carbon nanotubes (SWNTs), as they eventually determine the radiative and non-radiative recombination processes of generated carriers. In this work, we report systematic high-field magneto-optical study on the relative ordering between bright and dark excitons in SWNTs. We identified the relative energy position of the dark exciton unambiguously by brightening it in ultra-high magnetic field. The bright-dark excitonic ordering was found to depend not only on the tube structure, but also on the type of transitions. For the 1st sub-band transition, the bright exciton appears to be higher in energy than its dark counterpart for any chiral species and is robust against environmental effect. While for the 2nd sub-band, their relative ordering was found to be chirality-sensitive: the bright exciton can be either higher or lower than the dark one, depending on the specific nanotube structures. These findings provide new clues for engineering the optical and electronic properties of SWNTs. PMID:25385545
Relative ordering between bright and dark excitons in single-walled carbon nanotubes.
Zhou, Weihang; Nakamura, Daisuke; Liu, Huaping; Kataura, Hiromichi; Takeyama, Shojiro
2014-11-11
The ordering and relative energy splitting between bright and dark excitons are critical to the optical properties of single-walled carbon nanotubes (SWNTs), as they eventually determine the radiative and non-radiative recombination processes of generated carriers. In this work, we report systematic high-field magneto-optical study on the relative ordering between bright and dark excitons in SWNTs. We identified the relative energy position of the dark exciton unambiguously by brightening it in ultra-high magnetic field. The bright-dark excitonic ordering was found to depend not only on the tube structure, but also on the type of transitions. For the 1(st) sub-band transition, the bright exciton appears to be higher in energy than its dark counterpart for any chiral species and is robust against environmental effect. While for the 2(nd) sub-band, their relative ordering was found to be chirality-sensitive: the bright exciton can be either higher or lower than the dark one, depending on the specific nanotube structures. These findings provide new clues for engineering the optical and electronic properties of SWNTs.
NASA Astrophysics Data System (ADS)
Bardeen, Christopher J.
2016-09-01
The ability to downconvert (1 photon to 2 photons) and upconvert (2 photons to 1 photon) energy can boost solar energy conversion efficiencies by 30% or more. Downconversion can be accomplished through exciton fission, in which an initially created high energy singlet exciton spontaneously splits into a pair of lower energy triplet excitons. In organic semiconductors like tetracene and rubrene, the Frenkel character of the excitons leads to energetically separate singlet and triplet bands, providing an ideal set of energy levels for both processes to take place. In this talk, our efforts to understand the basic photophysics of singlet fission using time-resolved transient absorption, photoluminescence and magnetic field effects will be described. The role of molecular packing in controlling the fission rate will be emphasized. Upconversion occurs via the reverse process, where a pair of triplet excitons fuse into a high-energy singlet state. While most approaches to upconversion require a sensitizer to populate the dark triplet states, an alternate approach is to take advantage of low-energy intermolecular states in organic crystals to sensitize triplet states. We show that this process can be surprisingly efficient in certain molecular crystals, even in the absence of sensitizers. The exciton interactions responsible for this process are investigated using steady-state and time-resolved spectroscopy.
Zener Polarons Ordering Variants Induced by A-Site Ordering in Half-Doped Manganites
NASA Astrophysics Data System (ADS)
Daoud-Aladine, Aziz
2006-03-01
Zener Polaron (ZP) ordering [1] provides a still polemic [2] and elusive interpretation of the charge ordering (CO) phenomenon in A site disordered half doped (A1/2Ca1/2) MnO3, which is classically pictured by the Goodenough model (GM) of Mn^3+ and Mn^4+ CO [3,4]. ZP ordering considers instead the ordering of pre-formed ferromagnetic Mn pairs sharing an charge and keeping Mn in a Mn^+3.5 valence state. The recently synthesized A site cation ordered ABaMn2O6 were shown to not present the generic magnetic CE state found of (A1/2Ca1/2)MnO3 [5]. We present our magnetic structure determination of YBaMn2O6: the non- collinear magnetic order obtained unexpectedly reveals ferromagnetic plaquettes of four Mn attributable to larger 4-Mn ZPs, whose presence additionally fits very well the effective paramagnetic moments inferred from susceptibility measurements. The results unambiguously reveal the possible existence of ZP ordering variant in charge ordered manganites. [1] A. Daoud-Aladine et al., Phys. Rev. Lett. 89, 097205 (2002) [2] S. Grenier et al., Phys. Rev. B 69, 134419 (2004) [3] J. B. Goodenough, Phys. Rev. 100, 564 (1955) [4] P.G. Radaelli et al., Phys. Rev. B, 55, 3015 (1997) [5] T. Arima et al., Phys. Rev. B 66, 140408 (2002)
Exciton spin coherence in InGaAs/GaAs quantum dots revisited by heterodyne pump-probe experiment
NASA Astrophysics Data System (ADS)
Eble, B.; Siarry, B.; Bernardot, F.; Grinberg, P.; Testelin, C.; Lemaître, A.
2016-10-01
We demonstrate here the phase control of the neutral exciton quantum beats in InGaAs/GaAs quantum dots. A longitudinal magnetic field is used as a tuning parameter to change the phase of the oscillations in a deterministic way. This effect arises from the competition between the Zeeman splitting and the electron/hole exchange interaction on the exciton dipole symmetry. To explore this mechanism, we have developed a pump-probe setup based on the optical heterodyne detection of the quantum dots reflectivity allowing one to measure the exciton dynamics from a small quantum dots ensemble (˜300).
Bound exciton and free exciton states in GaSe thin slab
Wei, Chengrong; Chen, Xi; Li, Dian; Su, Huimin; He, Hongtao; Dai, Jun-Feng
2016-01-01
The photoluminescence (PL) and absorption experiments have been performed in GaSe slab with incident light polarized perpendicular to c-axis of sample at 10 K. An obvious energy difference of about 34 meV between exciton absorption peak and PL peak (the highest energy peak) is observed. By studying the temperature dependence of PL and absorption spectra, we attribute it to energy difference between free exciton and bound exciton states, where main exciton absorption peak comes from free exciton absorption, and PL peak is attributed to recombination of bound exciton at 10 K. This strong bound exciton effect is stable up to 50 K. Moreover, the temperature dependence of integrated PL intensity and PL lifetime reveals that a non-radiative process, with activation energy extracted as 0.5 meV, dominates PL emission. PMID:27654064
Bound exciton and free exciton states in GaSe thin slab
NASA Astrophysics Data System (ADS)
Wei, Chengrong; Chen, Xi; Li, Dian; Su, Huimin; He, Hongtao; Dai, Jun-Feng
2016-09-01
The photoluminescence (PL) and absorption experiments have been performed in GaSe slab with incident light polarized perpendicular to c-axis of sample at 10 K. An obvious energy difference of about 34 meV between exciton absorption peak and PL peak (the highest energy peak) is observed. By studying the temperature dependence of PL and absorption spectra, we attribute it to energy difference between free exciton and bound exciton states, where main exciton absorption peak comes from free exciton absorption, and PL peak is attributed to recombination of bound exciton at 10 K. This strong bound exciton effect is stable up to 50 K. Moreover, the temperature dependence of integrated PL intensity and PL lifetime reveals that a non-radiative process, with activation energy extracted as 0.5 meV, dominates PL emission.
The Influence of Surface Phonons on Polaron States in Quantum Dots
NASA Astrophysics Data System (ADS)
Maslov, A. Yu.; Proshina, O. V.; Rusina, A. N.
2007-04-01
The influence of the surface phonons on the polaron effect in a quantum dot is investigated. We consider the polar quantum dot embedded into the polar matrix. The polaron energy shift for the electron and hole ground states is calculated. It is shown that the contribution of the surface phonons may exceed the bulk phonon contribution.
Landau levels of the C-exciton in CuInSe{sub 2} studied by magneto-transmission
Yakushev, M. V.; Rodina, A. V.; Shuchalin, G. M.; Seisian, R. P.; Abdullaev, M. A.; Rockett, A.; Zhivulko, V. D.; Mudryi, A. V.; Faugeras, C.; Martin, R. W.
2014-10-06
The electronic structure of the solar cell absorber CuInSe{sub 2} is studied using magneto-transmission in thin polycrystalline films at magnetic fields up to 29 T. A, B, and C free excitons are resolved in absorption spectra at zero field and a Landau level fan generated by diamagnetic exciton recombination is observed for fields above 7 T. The dependence of the C band exciton binding energy on magnetic fields, calculated using a hydrogenic approximation, is used to determine the C exciton Rydberg at 0 T (8.5 meV), band gap (1.2828 eV), and hole effective mass m{sub so} = (0.31 ± 0.12)m{sub 0} for the C valence sub-band.
Exciton-polaritons condensate in a microwire
NASA Astrophysics Data System (ADS)
Kamoun, O.; Jaziri, S.
2013-12-01
Recently, polariton condensation has been claimed in microwires. Numerical solutions of the time-dependent Gross-Pitaevskii equation that describes the behavior of the condensate in a trap and exciton-polariton interaction, have been obtained. In this work we study theoretically exciton-polariton one dimensional condensation in several quantized states.
DNA-mediated excitonic upconversion FRET switching
Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; ...
2015-11-17
Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy up conversion via up conversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based up conversion has been demonstrated, it suffersmore » from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an up conversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy up conversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy up conversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.« less
DNA-mediated excitonic upconversion FRET switching
Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; Davis, Paul H.; Graugnard, Elton; Lee, Jeunghoon; Yurke, Bernard; Knowlton, William B.
2015-11-17
Excitonics is a rapidly expanding field of nanophotonics in which the harvesting of photons, ensuing creation and transport of excitons via Förster resonant energy transfer (FRET), and subsequent charge separation or photon emission has led to the demonstration of excitonic wires, switches, Boolean logic and light harvesting antennas for many applications. FRET funnels excitons down an energy gradient resulting in energy loss with each step along the pathway. Conversely, excitonic energy up conversion via up conversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based up conversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an up conversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy up conversion by nearly a factor of 2, an excited state donor to acceptor FRET efficiency of nearly 25%, and an acceptor fluorophore quantum efficiency that is close to unity. These findings offer a promising path for energy up conversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.
NASA Astrophysics Data System (ADS)
Dinh, Van An; Nara, Jun; Ohno, Takahisa
2012-04-01
Based on the Heyd-Scuseria-Ernzerhof hybrid density functionals study, we proposed a new insight into the diffusion of polaron-Li vacancy complexes in LiFe1-yMnyPO4 (y=0,1/2,1). It is found that the polaron migrates along a crossing or a parallel path relative to the Li moving direction. In LiFePO4, the complex diffusion along the zigzag pathway is favorable and has a barrier of 600 meV, while the diffusion along the parallel pathway with a barrier of 623 meV is favorable in LiMnPO4. For LiFe1/2Mn1/2PO4, since the polaron is formed within a single Fe layer, the diffusion proceeds along the parallel pathway with a barrier of 635 meV.
Superexchange coupling and electron transfer in globular proteins via polaron excitations.
Chuev, G N; Lakhno, V D; Ustitnin, M N
1999-06-01
The polaron approach is used to treat long-range electron transfers between globular proteins. A rate expression for the polaron transfer model is given along with a description of appropriate conditions for its use. Assuming that electrons transfer via a superexchange coupling due to a polaron excitation, we have estimated the distance dependence of the rate constant for the self-exchange reactions between globular proteins in solutions. The distance dependence of the polaron coupling and solvent reorganization energy are provided as a basis for understanding and interpreting a long-range electron transfer experiment. The difficulties and problems of the polaron treatment of long-range electron transfers are discussed, and suggestions for new experiments are made.
Excitons and optical spectra of phosphorene nanoribbons
NASA Astrophysics Data System (ADS)
Nourbakhsh, Zahra; Asgari, Reza
2016-07-01
On the basis of many-body ab initio calculations, using the single-shot G0W0 method and Bethe-Salpeter equation, we study phosphorene nanoribbons (PNRs) in the two typical zigzag and armchair directions. The electronic structure, optical absorption, electron-hole (exciton) binding energy, exciton exchange splitting, and exciton wave functions are calculated for different sizes of PNRs. The typically strong splitting between singlet and triplet excitonic states make PNRs favorable systems for optoelectronic applications. Quantum confinement occurs in both kinds of PNRs, and it is stronger in the zPNRs, which behave like quasi-zero-dimensional systems. Scaling laws are investigated for the size-dependent behaviors of PNRs. The first bright excitonic state in PNRs is explored in detail.
Excitonic energy transfer in light-harvesting complexes in purple bacteria.
Ye, Jun; Sun, Kewei; Zhao, Yang; Yu, Yunjin; Lee, Chee Kong; Cao, Jianshu
2012-06-28
Two distinct approaches, the Frenkel-Dirac time-dependent variation and the Haken-Strobl model, are adopted to study energy transfer dynamics in single-ring and double-ring light-harvesting (LH) systems in purple bacteria. It is found that the inclusion of long-range dipolar interactions in the two methods results in significant increase in intra- or inter-ring exciton transfer efficiency. The dependence of exciton transfer efficiency on trapping positions on single rings of LH2 (B850) and LH1 is similar to that in toy models with nearest-neighbor coupling only. However, owing to the symmetry breaking caused by the dimerization of BChls and dipolar couplings, such dependence has been largely suppressed. In the studies of coupled-ring systems, both methods reveal an interesting role of dipolar interactions in increasing energy transfer efficiency by introducing multiple intra/inter-ring transfer paths. Importantly, the time scale (4 ps) of inter-ring exciton transfer obtained from polaron dynamics is in good agreement with previous studies. In a double-ring LH2 system, non-nearest neighbor interactions can induce symmetry breaking, which leads to global and local minima of the average trapping time in the presence of a non-zero dephasing rate, suggesting that environment dephasing helps preserve quantum coherent energy transfer when the perfect circular symmetry in the hypothetic system is broken. This study reveals that dipolar coupling between chromophores may play an important role in the high energy transfer efficiency in the LH systems of purple bacteria and many other natural photosynthetic systems.
Excitonic energy transfer in light-harvesting complexes in purple bacteria
Ye Jun; Sun Kewei; Zhao Yang; Lee, Chee Kong; Yu Yunjin; Cao Jianshu
2012-06-28
Two distinct approaches, the Frenkel-Dirac time-dependent variation and the Haken-Strobl model, are adopted to study energy transfer dynamics in single-ring and double-ring light-harvesting (LH) systems in purple bacteria. It is found that the inclusion of long-range dipolar interactions in the two methods results in significant increase in intra- or inter-ring exciton transfer efficiency. The dependence of exciton transfer efficiency on trapping positions on single rings of LH2 (B850) and LH1 is similar to that in toy models with nearest-neighbor coupling only. However, owing to the symmetry breaking caused by the dimerization of BChls and dipolar couplings, such dependence has been largely suppressed. In the studies of coupled-ring systems, both methods reveal an interesting role of dipolar interactions in increasing energy transfer efficiency by introducing multiple intra/inter-ring transfer paths. Importantly, the time scale (4 ps) of inter-ring exciton transfer obtained from polaron dynamics is in good agreement with previous studies. In a double-ring LH2 system, non-nearest neighbor interactions can induce symmetry breaking, which leads to global and local minima of the average trapping time in the presence of a non-zero dephasing rate, suggesting that environment dephasing helps preserve quantum coherent energy transfer when the perfect circular symmetry in the hypothetic system is broken. This study reveals that dipolar coupling between chromophores may play an important role in the high energy transfer efficiency in the LH systems of purple bacteria and many other natural photosynthetic systems.
Two-Dimensional Polaronic Behavior in the Binary Oxides m-HfO2 and m-ZrO2
Mckenna, Keith P.; Wolf, Matthew J.; Shluger, Alexander L.; Lany, Stephan; Zunger, Alex
2012-03-14
We demonstrate that the three-dimensional (3D) binary monoclinic oxides HfO2 and ZrO2 exhibit quasi-2D polaron localization and conductivity, which results from a small difference in the coordination of two oxygen sublattices in these materials. The transition between a 2D large polaron into a zerodimensional small polaron state requires overcoming a small energetic barrier. These results demonstrate how a small asymmetry in the lattice structure can determine the qualitative character of polaron localization and significantly broaden the realm of quasi-2D polaron systems.
Bilayer manganites: polarons in the midst of a metallic breakdown
NASA Astrophysics Data System (ADS)
Golden, Mark; Massee, Freek; de Jong, Sanne; Huang, Yingkai; Boothroyd, Andrew; Prabhakaran, D.; Follath, Rolf; Varykhalov, Andrei; Patthey, Luc; Shi, Ming; Goedkoop, Jeroen
2011-03-01
The exact nature of the low temperature electronic phase of the manganite materials family, and hence the origin of their colossal magnetoresistive (CMR) transition is still a flagship issue in emergent correlated matter research. By combining new photoemission and tunneling data, we show that in the bilayer (N = 2) manganite La 2-2x Sr 1+2x Mn 2 O7 the lattice/spin/orbital polaronic degrees of freedom win out, all across the CMR region of the phase diagram. This means that the generic ground state is that of a system in which strong interactions result in vanishing coherent quasi--particle spectral weight at the Fermi level for all locations in k --space. The incoherence of the charge carriers offers a unifying explanation for the anomalous charge-carrier dynamics seen in transport, optics and electron spectroscopic data. The stacking number N is the key factor for true metallic behavior, as an intergrowth-driven breakdown of the polaronic domination to give a robust metal possessing a traditional Fermi surface is seen in the bilayer system.
Spectroscopic Evidence of Formation of Small Polarons in Doped Manganites
NASA Astrophysics Data System (ADS)
Moritomo, Yutaka; Machida, Akihiko; Nakamura, Arao
1998-03-01
Temperature dependence of absorption spectra for thin films of doped manganites R_0.6Sr_0.4MnO_3, where R is rare-earth atom, has been investigated systematically changing averaged ionic radius < rA > of perovskite A-site. We have observed a specific absorption band at ~1.5eV due to optical excitations from small polarons (SP)(Machida et al.), submitted.. Spectral weight of the SP band increases with decreasing temperature and eventually disappears at the insulator-metal (IM) transition, indicating that SP in the paramagnetic state (T >= T_C) changes into bare electrons (or large polarons) in the ferromagnetic state due to the enhanced one-electron bandwidth W. We further derived important physical quantities, i.e., W, on-site exchange interaction J and binding energy Ep of SP, and discuss material dependence of stability of SP. This work was supported by a Grant-In-Aid for Scientific Research from the Ministry of Education, Science, Sport and Culture and from PRESTO, Japan Scienece and Technology Corporation (JST), Japan.
Excitonic polaritons of zinc diarsenide single crystals
NASA Astrophysics Data System (ADS)
Syrbu, N. N.; Stamov, I. G.; Zalamai, V. V.; Dorogan, A.
2017-02-01
Excitonic polaritons of ZnAs2 single crystals had been investigated. Parameters of singlet excitons with D2bar(z) symmetry and orthoexcitons 2D1bar(y)+D2bar(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 (V1) and electron (C1) bands. The values of effective masses of electrons (mc*=0.10 m0) and holes (mv1*=0.89 m0) had been estimated. It was revealed that the hole mass mv1* changes from 1.03 m0 to 0.55 m0 at temperature increasing from 10 K up to 230 K and that the electron mass mc* does not depend on temperature. The integral absorption A (eV cm-1) of the states n=1, 2 and 3 of D2bar(z) excitons depends on the An≈n-3 equality, which it is characteristic for S-type excitonic functions. Temperature dependences of the integral absorption of ground states for D2bar(z) and D2bar(D) excitons differ. The ground states of B and C excitons formed by V3 - C1 and V4 - C1 bands and its parameters had been determined.
NASA Astrophysics Data System (ADS)
Li, Zhi-xin; Wang, Xiao-yu
2016-12-01
On the basis of Lee-Low-Pines unitary transformation, the influences of Rashba spin-orbit (RSO) coupling energy and Zeeman splitting energy on the ground-state energy of polaron in a quantum rod (QRD) have been studied by using a variational method of Pekar type. Taking the RSO interaction and the Zeeman splitting into account, we derive the variational relations of the absolute ratios ζ1 and ζ2 of the RSO coupling energy and the Zeeman splitting energy to the ground-state energy of polaron with the transverse confinement radius (TCR) and the longitudinal confinement length (LCL) of QRD, as well as and the magnetic field adjusting length (MFAL). The results show that the absolute ratios ζ1 and ζ2 will increase when the TCR and the LCL become larger, but will slowly decrease while the MFAL and the aspect ratio of the ellipsoid δ increase, respectively. The above results can be attributed to the spin effects and interesting quantum size confining.
Ultracold Gas of Excitons in Traps
2012-06-08
Excitons in a GaAs Quantum-Well Structurewith a Diamond-Shaped Electrostatic Trap, Physical Review Letters, (08 2009): 87403. doi: 2012/06/08 14:38:06 19...Kinetics of the inner ring in the exciton emission pattern in coupled GaAs quantum wells, Physical Review B, (10 2009): 155331. doi: 2012/06/08 14:28:30...17 Sen Yang, , L. V. Butov, , L. S. Levitov, , B. D. Simons,, A. C. Gossard. Exciton front propagation in photoexcited GaAs quantum wells, Physical
Magnetic Studies of Photovoltaic Processes in Organic Solar Cells
Zang, Huidong; Ivanov, Ilia N; Hu, Bin
2010-01-01
In this paper, we use magnetic field effects of photocurrent (MFEPC ) to study the photovoltaic processes in pristine conjugated polymer, bulk heterojunction, and double-layer solar cells, respectively, based on poly(3-alkylthiophene) (P3HT). The MFEPC reveals that the photocurrent generation undergoes the dissociation in polaron pair states and the charge reaction in excitonic states in pristine conjugated polymers. As for the bulk-heterojunction solar cells consisting of electron donor P3HT and electron acceptor [6,6]-phenyl C61-butyric acid methyl ester (PCBM), the MFEPC indicates that the dissociated electrons and holes inevitably form the intermolecular charge-transfer (CT) complexes at donor and acceptor interfaces. Essentially, the photocurrent generation relies on the further dissociation of intermolecular CT complexes. Moreover, we use double-layer solar cell to further study the intermolecular CT complexes with well-controlled donor acceptor interfaces based on double-layer P3HT/TiOx design. We find that the increase in free energies can significantly reduce the density of CT complexes upon thermal annealing.
Influence of lithium vacancies on the polaronic transport in olivine phosphate structure
Murugavel, Sevi Sharma, Monika; Shahid, Raza
2016-01-28
Intercalation and deintercalation of lithium ions in cathode materials are of principal to the operation of current rechargeable lithium ion batteries. The performance of lithium ion batteries highly relies on the active cathode material which includes cell potential, power/energy density, capacity, etc. An important issue in this class of material is to resolve the factors governing the electron and ion transport in olivine phosphate structure. In this class of material, there is still an open debate on the mechanism of charge transport including both polarons and lithium ions. On the one hand, this is due to the large disparity between the experimental results and the theoretical model predictions. On the other hand, this is also due to the lack of precise experimental measurement without any parasitic phases in a given cathode material. Here, we present the polaronic conduction in lithiated triphylite LiFePO{sub 4} (LFP) and delithiated heterosite FePO{sub 4} (FP) by means of broadband ac impedance spectroscopy over wide range temperatures and frequency. It is found that the LFP phase possess two orders of higher polaronic conductivity than FP phase despite having similar mobility of polarons in both phases. We show that the differences in the polaronic conductivity of two phases are due to the significant differences in concentration of polarons. It is found that the formation energy of polarons in individual phases is mainly determined by the corresponding defect state associated with it. The temperature dependent dc conductivity has been analyzed within the framework of Mott model of polaronic conduction and explored the origin of polaronic conduction mechanism in this class of material.
Magneto-optical properties of Rydberg excitons: Center-of-mass quantization approach
NASA Astrophysics Data System (ADS)
Zielińska-Raczyńska, Sylwia; Ziemkiewicz, David; Czajkowski, Gerard
2017-02-01
We show how to compute the magneto-optical functions (absorption, reflection, and transmission) when Rydberg exciton polaritons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field, and the polaritonic effect. Using the real density-matrix approach the analytical expressions for magneto-optical functions are obtained and numerical calculations for Cu2O crystal are performed. The influence of the strength of applied external magnetic field on the resonance displacement of excitonic spectra is discussed. We report a good agreement with recently published experimental data.
Exciton storage in type-II quantum dots using the optical Aharonov-Bohm effect
Climente, Juan I.; Planelles, Josep
2014-05-12
We investigate the bright-to-dark exciton conversion efficiency in type-II quantum dots subject to a perpendicular magnetic field. To this end, we take the exciton storage protocol recently proposed by Simonin and co-workers [Phys. Rev. B 89, 075304 (2014)] and simulate its coherent dynamics. We confirm the storage is efficient in perfectly circular structures subject to weak external electric fields, where adiabatic evolution is dominant. In practice, however, the efficiency rapidly degrades with symmetry lowering. Besides, the use of excited states is likely unfeasible owing to the fast decay rates. We then propose an adaptation of the protocol which does not suffer from these limitations.
Acoustic-excitonic effects in a two-dimensional gas of dipolar excitons
NASA Astrophysics Data System (ADS)
Boev, M. V.; Kovalev, V. M.; Chaplik, A. V.
2016-08-01
The theory of the interaction of a two-dimensional gas of indirect dipolar excitons with Rayleigh surface elastic waves has been developed. The absorption and renormalization of the phase velocity of a surface wave, as well as the drag of excitons by the surface acoustic wave and the generation of bulk acoustic waves by a twodimensional gas of dipolar excitons irradiated by external electromagnetic radiation, have been considered. These effects have been studied both in a normal phase at high temperatures and in a condensed phase of the exciton gas. The calculations have been performed in the ballistic and diffusion limits for both phases.
Optical nutation in the exciton range of spectrum
Khadzhi, P. I.; Vasiliev, V. V.
2013-08-15
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.
Excitons in boron nitride single layer
NASA Astrophysics Data System (ADS)
Galvani, Thomas; Paleari, Fulvio; Miranda, Henrique P. C.; Molina-Sánchez, Alejandro; Wirtz, Ludger; Latil, Sylvain; Amara, Hakim; Ducastelle, François
2016-09-01
Boron nitride single layer belongs to the family of two-dimensional materials whose optical properties are currently receiving considerable attention. Strong excitonic effects have already been observed in the bulk and still stronger effects are predicted for single layers. We present here a detailed study of these properties by combining ab initio calculations and a tight-binding Wannier analysis in both real and reciprocal space. Due to the simplicity of the band structure with single valence (π ) and conduction (π*) bands the tight-binding analysis becomes quasiquantitative with only two adjustable parameters and provides tools for a detailed analysis of the exciton properties. Strong deviations from the usual hydrogenic model are evidenced. The ground-state exciton is not a genuine Frenkel exciton, but a very localized tightly bound one. The other ones are similar to those found in transition-metal dichalcogenides and, although more localized, can be described within a Wannier-Mott scheme.
Radiative lifetime of excitons in carbon nanotubes.
Perebeinos, Vasili; Tersoff, J; Avouris, Phaedon
2005-12-01
We calculate the radiative lifetime and energy bandstructure of excitons in semiconducting carbon nanotubes within a tight-binding approach including the electron-hole correlations via the Bethe-Salpeter equation. In the limit of rapid interband thermalization, the radiative decay rate is maximized at intermediate temperatures and decreases at low temperature because the lowest-energy excitons are optically forbidden. The intrinsic phonons cannot scatter excitons between optically active and forbidden bands, so sample-dependent extrinsic effects that break the symmetries can play a central role. We calculate the diameter-dependent energy splittings between singlet and triplet excitons of different symmetries and the resulting dependence of radiative lifetime on temperature and tube diameter.
Probing dark exciton diffusion using photovoltage
Mullenbach, Tyler K.; Curtin, Ian J.; Zhang, Tao; Holmes, Russell J.
2017-01-01
The migration of weakly and non-luminescent (dark) excitons remains an understudied subset of exciton dynamics in molecular thin films. Inaccessible via photoluminescence, these states are often probed using photocurrent methods that require efficient charge collection. Here we probe exciton harvesting in both luminescent and dark materials using a photovoltage-based technique. Transient photovoltage permits a real-time measurement of the number of charges in an organic photovoltaic cell, while avoiding non-geminate recombination losses. The extracted exciton diffusion lengths are found to be similar to those determined using photocurrent. For the luminescent material boron subphthalocyanine chloride, the photovoltage determined diffusion length is less than that extracted from photoluminescence. This indicates that while photovoltage circumvents non-geminate losses, geminate recombination at the donor–acceptor interface remains the primary recombination pathway. Photovoltage thus offers a general approach for extracting a device-relevant diffusion length, while also providing insight in to the dominant carrier recombination pathways. PMID:28128206
Probing dark exciton diffusion using photovoltage
NASA Astrophysics Data System (ADS)
Mullenbach, Tyler K.; Curtin, Ian J.; Zhang, Tao; Holmes, Russell J.
2017-01-01
The migration of weakly and non-luminescent (dark) excitons remains an understudied subset of exciton dynamics in molecular thin films. Inaccessible via photoluminescence, these states are often probed using photocurrent methods that require efficient charge collection. Here we probe exciton harvesting in both luminescent and dark materials using a photovoltage-based technique. Transient photovoltage permits a real-time measurement of the number of charges in an organic photovoltaic cell, while avoiding non-geminate recombination losses. The extracted exciton diffusion lengths are found to be similar to those determined using photocurrent. For the luminescent material boron subphthalocyanine chloride, the photovoltage determined diffusion length is less than that extracted from photoluminescence. This indicates that while photovoltage circumvents non-geminate losses, geminate recombination at the donor-acceptor interface remains the primary recombination pathway. Photovoltage thus offers a general approach for extracting a device-relevant diffusion length, while also providing insight in to the dominant carrier recombination pathways.
Exciton absorption in narrow armchair graphene nanoribbons
NASA Astrophysics Data System (ADS)
Monozon, B. S.; Schmelcher, P.
2016-11-01
We develop an analytical approach to the exciton optical absorption for narrow gap armchair graphene nanoribbons (AGNR). We focus on the regime of dominant size quantization in combination with the attractive electron-hole interaction. An adiabatic separation of slow and fast motions leads via the two-body Dirac equation to the isolated and coupled subband approximations. Discrete and continuous exciton states are in general coupled and form quasi-Rydberg series of purely discrete and resonance type character. The corresponding oscillator strengths and widths are derived. We show that the exciton peaks are blue-shifted, become broader and increase in magnitude upon narrowing the ribbon. At the edge of a subband the singularity related to the 1D density of states is transformed into finite absorption via the presence of the exciton. Our analytical results are in good agreement with those obtained by other methods including numerical approaches. Estimates of the expected experimental values are provided for realistic AGNR.
Signatures of Quantum Coherences in Rydberg Excitons
NASA Astrophysics Data System (ADS)
Grünwald, P.; Aßmann, M.; Heckötter, J.; Fröhlich, D.; Bayer, M.; Stolz, H.; Scheel, S.
2016-09-01
Coherent optical control of individual particles has been demonstrated both for atoms and semiconductor quantum dots. Here we demonstrate the emergence of quantum coherent effects in semiconductor Rydberg excitons in bulk Cu2O . Because of the spectral proximity between two adjacent Rydberg exciton states, a single-frequency laser may pump both resonances with little dissipation from the detuning. As a consequence, additional resonances appear in the absorption spectrum that correspond to dressed states consisting of two Rydberg exciton levels coupled to the excitonic vacuum, forming a V -type three-level system, but driven only by one laser light source. We show that the level of pure dephasing in this system is extremely low. These observations are a crucial step towards coherently controlled quantum technologies in a bulk semiconductor.
Exciton-polariton wakefields in semiconductor microcavities
NASA Astrophysics Data System (ADS)
Terças, H.; Mendonça, J. T.
2016-02-01
We consider the excitation of polariton wakefields due to a propagating light pulse in a semiconductor microcavity. We show that two kinds of wakes are possible, depending on the constituents fraction (either exciton or photon) of the polariton wavefunction. The nature of the wakefields (pure excitonic or polaritonic) can be controlled by changing the speed of propagation of the external pump. This process could be used as a diagnostic for the internal parameters of the microcavity.
Exciton properties of selected aromatic hydrocarbon systems
NASA Astrophysics Data System (ADS)
Roth, Friedrich; Mahns, Benjamin; Hampel, Silke; Nohr, Markus; Berger, Helmuth; Büchner, Bernd; Knupfer, Martin
2013-02-01
We have examined the singlet excitons in two representatives of acene-type (tetracene and pentacene) and phenacene-type (chrysene and picene) molecular crystals, respectively, using electron energy-loss spectroscopy at low temperatures. We show that the excitation spectra of the two hydrocarbon families significantly differ. Moreover, close inspection of the data indicates that there is an increasing importance of charge-transfer excitons at lowest excitation energy with increasing length of the molecules.
Ultrafast exciton dynamics at molecular surfaces
NASA Astrophysics Data System (ADS)
Monahan, Nicholas R.
Further improvements to device performance are necessary to make solar energy conversion a compelling alternative to fossil fuels. Singlet exciton fission and charge separation are two processes that can heavily influence the power conversion efficiency of a solar cell. During exciton fission one singlet excitation converts into two triplet excitons, potentially doubling the photocurrent generated by higher energy photons. There is significant discord over the singlet fission mechanism and of particular interest is whether the process involves a multiexciton intermediate state. I used time-resolved two-photon photoemission to investigate singlet fission in hexacene thin films, a model system with strong electronic coupling. My results indicate that a multiexciton state forms within 40 fs of photoexcitation and loses singlet character on a 280 fs timescale, creating two triplet excitons. This is concordant with the transient absorption spectra of hexacene single crystals and definitively proves that exciton fission in hexacene proceeds through a multiexciton state. This state is likely common to all strongly-coupled systems and my results suggest that a reassessment of the generally-accepted singlet fission mechanism is required. Charge separation is the process of splitting neutral excitons into carriers that occurs at donor-acceptor heterojunctions in organic solar cells. Although this process is essential for device functionality, there are few compelling explanations for why it is highly efficient in certain organic photovoltaic systems. To investigate the charge separation process, I used the model system of charge transfer excitons at hexacene surfaces and time-resolved two-photon photoemission. Charge transfer excitons with sufficient energy spontaneously delocalize, growing from about 14 nm to over 50 nm within 200 fs. Entropy drives this delocalization, as the density of states within the Coulomb potential increases significantly with energy. This charge
Bose polaron problem: Effect of mass imbalance on binding energy
NASA Astrophysics Data System (ADS)
Ardila, L. A. Peña; Giorgini, S.
2016-12-01
By means of quantum Monte Carlo methods we calculate the binding energy of an impurity immersed in a Bose-Einstein condensate at T =0 . The focus is on the attractive branch of the Bose polaron and on the role played by the mass imbalance between the impurity and the surrounding particles. For an impurity resonantly coupled to the bath, we investigate the dependence of the binding energy on the mass ratio and on the interaction strength within the medium. In particular, we determine the equation of state in the case of a static (infinite mass) impurity, where three-body correlations are irrelevant and the result is expected to be a universal function of the gas parameter. For the mass ratio corresponding to 40K impurities in a gas of 87Rb atoms, we provide an explicit comparison with the experimental findings of a recent study carried out at JILA.
Polaron transport in TiO{sub 2} thin films
Yildiz, Abdullah; Iacomi, Felicia; Mardare, Diana
2010-10-15
Undoped and Fe-doped TiO{sub 2} thin films were obtained by rf-sputtering technique onto heated glass substrates (250 deg. C) covered with indium tin oxide. The temperature dependence of the electrical conductivity was investigated in the temperature range 13-320 K, and it shows that the conduction mechanism in the studied samples is described by small-polaron hopping (SPH) at temperatures higher than half of the Debye temperature ({theta}{sub D}). It was found that the magnitude of the SPH coupling increases by Fe doping in TiO{sub 2} thin films. With decreasing temperature, the conduction behavior transited from SPH conduction to variable-range hopping (VRH) conduction. In the intermediate temperature domain (200 K
Exciton Resonances in Novel Silicon Carbide Polymers
NASA Astrophysics Data System (ADS)
Burggraf, Larry; Duan, Xiaofeng
2015-05-01
A revolutionary technology transformation from electronics to excitionics for faster signal processing and computing will be advantaged by coherent exciton transfer at room temperature. The key feature required of exciton components for this technology is efficient and coherent transfer of long-lived excitons. We report theoretical investigations of optical properties of SiC materials having potential for high-temperature excitonics. Using Car-Parinello simulated annealing and DFT we identified low-energy SiC molecular structures. The closo-Si12C12 isomer, the most stable 12-12 isomer below 1100 C, has potential to make self-assembled chains and 2-D nanostructures to construct exciton components. Using TDDFT, we calculated the optical properties of the isomer as well as oligomers and 2-D crystal formed from the isomer as the monomer unit. This molecule has large optical oscillator strength in the visible. Its high-energy and low-energy transitions (1.15 eV and 2.56 eV) are nearly pure one-electron silicon-to-carbon transitions, while an intermediate energy transition (1.28 eV) is a nearly pure carbon-to-silicon one-electron charge transfer. These results are useful to describe resonant, coherent transfer of dark excitons in the nanostructures. Research supported by the Air Force Office of Scientific Research.
Hybrid functional studies of defects and hole polarons in oxides
NASA Astrophysics Data System (ADS)
Varley, Joel
Transparent conducting oxides (TCOs) are ubiquitous, appearing in windows, flat-panel displays, solar cells, solid-state lighting, and transistors that all exploit TCOs' combination of high electrical conductivity and optical transparency. Thanks to this large and growing list of applications, there has been a surge of interest in the science of these materials, focusing on the fundamental properties and doping opportunities in traditional TCOs as well as the exploration of promising new candidate materials. Hybrid density functional theory has proven instrumental in elucidating the physics of TCOs. One example is the study of dopants and defects that determine the conductivity. Accurate formation energies and charge-state transition levels can now be obtained thanks to the accurate electronic structure provided by a hybrid functional. This allows us to address the origins of unintentional conductivity: for SnO2, In2O3, and Ga2O3, we demonstrate that this is not due to native defects such as oxygen vacancies, but must be attributed to unintentional incorporation of impurities. We can also provide guidelines for achieving higher doping levels, suggesting several impurities as candidate donors with high solubility. Limitations on doping due to the formation or incorporation of compensating centers are addressed as well. Hybrid functional calculations also overcome the shortcomings associated with traditional local or semi-local functionals, which do not properly describe charge localization. Hybrid functionals accurately describe polaron formation, i.e., the self-trapping of holes when p - type doping of the oxide materials is attempted. Consequences of polaron formation for optical characterization of the material will be discussed. This work was performed in collaboration with Anderson Janotti and Chris G. Van de Walle, and was in part under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.
Dynamics of light-induced NIR-absorption of Nb4 polarons in SBN
NASA Astrophysics Data System (ADS)
Gao, Ming; Vikhnin, V.; Kapphan, S.
The dynamics of light-induced (Kr+-, Ar+-laser) electronic polarons (Nb4+ centers with broad absorption band around 0.8 eV) and light-induced centers of other types were investigated in SrxBa1-xNb2O6: Cr (SBN:Cr) and in SBN: Ce using FTIR absorption measurements at low temperature. A theoretical model involving Cr3+/Cr4+, Ce3+/Ce4+, Nb4+ electronic polarons and trapping X-centers is proposed. The trapping of polarons at Cr4+/Ce4+ centers with subsequent recharging is shown to play an important role in the polaron dynamics. The predictions of the model are in very good agreement with the experimental results.
Formation and local symmetry of the Holstein polaron in the t-J model
NASA Astrophysics Data System (ADS)
Ma, Han; Lee, T. K.; Chen, Yan
2013-04-01
The formation and local symmetry of a spin-lattice polaron has been investigated semiclassically in planar Holstein t-J-like models within the exact diagonalization method. Due to the interplay of strong correlations and electron-lattice interaction, the doped hole may either move freely or lead to the localized spin-lattice distortion and form a Holstein polaron. The formation of a polaron breaks the translational symmetry by suppression of antiferromagnetic correlations and inducement of ferromagnetic correlations locally. Moreover, the breaking of local rotational symmetry around the polaron has been shown. The ground state is generically a parity singlet and the first excited state may be a parity doublet. Further consequences of the density of states spectra for comparison with scanning tunneling microscopy experiments are discussed.
Interaction of Dirac Fermion excitons and biexciton-exciton cascade in graphene quantum dots
NASA Astrophysics Data System (ADS)
Ozfidan, Isil; Korkusinski, Marek; Hawrylak, Pawel
2015-03-01
We present a microscopic theory of interacting Dirac quasi-electrons and quasi-holes confined in graphene quantum dots. The single particle states of quantum dots are described using a tight binding model and screened direct, exchange, and scattering Coulomb matrix elements are computed using Slater pz orbitals. The many-body ground and excited states are expanded in a finite number of electron-hole pair excitations from the Hartree-Fock ground state and computed using exact diagonalization techniques. The resulting exciton and bi-exciton spectrum reflects the degeneracy of the top of the valence and bottom of the conduction band characteristic of graphene quantum dots with C3 symmetry. We study the interaction of multi-electron and hole complexes as a function of quantum dot size, shape and strength of Coulomb interactions. We identify two degenerate bright exciton (X) states and a corresponding biexciton (XX) state as XX-X cascade candidates, a source of entangled photon pairs. We next calculate the exciton to bi-exciton transitions detected in transient absorption experiments to extract the strength of exciton-exciton interactions and biexciton binding energies. We further explore the possibility of excitonic instability.
[Long-range electron transfer in globular proteins by polaron excitation].
Lakhno, V L; Chuev, G N
1997-01-01
Considering polaron model, we have calculated an electron state localized in the protein heme. Using these calculations: the electron density and electron energy, we estimated the self-exchange rate constant for cyt c (horse heart), its reorganization energy, matrix element, and dependence of this rate on the distance between hemes. The results are compared with the experimental data and other theoretical estimations. We discuss the role of polaron excitations in the long-range electron transfer in globular proteins.
Infrared absorption spectra of molecular crystals: Possible evidence for small-polaron formation?
NASA Astrophysics Data System (ADS)
Pržulj, Željko; Čevizović, Dalibor; Zeković, Slobodan; Ivić, Zoran
2008-09-01
The temperature dependence of the position of the so-called anomalous band peaked at 1650cm in the IR-absorption spectrum of crystalline acetanilide (ACN) is theoretically investigated within the small-polaron theory. Its pronounced shift towards the position of the normal band is predicted with the rise of temperature. Interpretation of the IR-absorption spectra in terms of small-polaron model has been critically assessed on the basis of these results.
Yan, Yun-An
2016-01-14
The quantum interference is an intrinsic phenomenon in quantum physics for photon and massive quantum particles. In principle, the quantum interference may also occur with quasi-particles, such as the exciton. In this study, we show how the exciton quantum interference can be significant in aggregates through theoretical simulations with hierarchical equations of motion. The systems under investigation are generalized donor-bridge-acceptor model aggregates with the donor consisting of six homogeneous sites assuming the nearest neighbor coupling. For the models with single-path bridge, the exciton transfer time only shows a weak excitation energy dependence. But models with double-path bridge have a new short transfer time scale and the excitation energy dependence of the exciton transfer time assumes clear peak structure which is detectable with today’s nonlinear spectroscopy. This abnormality is attributed to the exciton quantum interference and the condition for a clear observation in experiment is also explored.
Exciton polarizability in semiconductor nanocrystals.
Wang, Feng; Shan, Jie; Islam, Mohammad A; Herman, Irving P; Bonn, Mischa; Heinz, Tony F
2006-11-01
The response of charge to externally applied electric fields is an important basic property of any material system, as well as one critical for many applications. Here, we examine the behaviour and dynamics of charges fully confined on the nanometre length scale. This is accomplished using CdSe nanocrystals of controlled radius (1-2.5 nm) as prototype quantum systems. Individual electron-hole pairs are created at room temperature within these structures by photoexcitation and are probed by terahertz (THz) electromagnetic pulses. The electronic response is found to be instantaneous even for THz frequencies, in contrast to the behaviour reported in related measurements for larger nanocrystals and nanocrystal assemblies. The measured polarizability of an electron-hole pair (exciton) amounts to approximately 10(4) A(3) and scales approximately as the fourth power of the nanocrystal radius. This size dependence and the instantaneous response reflect the presence of well-separated electronic energy levels induced in the system by strong quantum-confinement effects.
Diagrammatic Monte Carlo study of mass-imbalanced Fermi-polaron system
NASA Astrophysics Data System (ADS)
Pollet, Lode
After a brief introduction and review of diagrammatic Monte Carlo, I present our results for the three-dimensional Fermi-polaron system with mass-imbalance, where an impurity interacts resonantly with a noninteracting Fermi sea whose atoms have a different mass. This method allows to go beyond frequently used variational techniques by stochastically summing all relevant impurity Feynman diagrams up to a maximum expansion order limited by the sign problem. The polaron energy and quasiparticle residue can be accurately determined over a broad range of impurity masses. Furthermore, the spectral function of an imbalanced polaron demonstrates the stability of the quasiparticle and allows to locate in addition also the repulsive polaron as an excited state. The quantitative exactness of two-particle-hole wave-functions is investigated, resulting in a relative lowering of polaronic energies in the mass-imbalance phase diagram. Tan's contact coefficient for the mass-balanced polaron system is found in good agreement with variational methods. Mass-imbalanced systems can be studied experimentally by ultracold atom mixtures like 6Li-40K. I will discuss some open questions and links with recent experiments.
Diagrammatic Monte Carlo study of a mass-imbalanced Fermi-polaron system
NASA Astrophysics Data System (ADS)
Kroiss, Peter; Pollet, Lode
2015-04-01
We apply the diagrammatic Monte Carlo approach to three-dimensional Fermi-polaron systems with mass imbalance, where an impurity interacts resonantly with a noninteracting Fermi sea whose atoms have a different mass. This method allows us to go beyond frequently used variational techniques by stochastically summing all relevant impurity Feynman diagrams up to a maximum expansion order limited by the sign problem. Polaron energy and quasiparticle residue can be accurately determined over a broad range of impurity masses. Furthermore, the spectral function of an imbalanced polaron demonstrates the stability of the quasiparticle and allows us to locate in addition also the repulsive polaron as an excited state. The quantitative exactness of two-particle-hole wave functions is investigated, resulting in a relative lowering of polaronic energies in the mass-imbalance phase diagram. Tan's contact coefficient for the mass-balanced polaron system is found in good agreement with variational methods. Mass-imbalanced systems can be studied experimentally by ultracold atom mixtures such as 6Li-40K.
Exciton transport and dissociation at organic interfaces
NASA Astrophysics Data System (ADS)
Beljonne, David
2011-03-01
This paper focuses on modeling studies of exciton transport and dissociation at organic interfaces and includes three parts: 1) Experiments have shown that the values of exciton diffusion length LD in conjugated polymers (CPs) are rather low, in the range of 5-10 nm, apparently regardless of their chemical structure and solid-state packing. In contrast, larger LD values have been reported in molecular materials that are chemically more well-defined than CPs. Here we demonstrate that energetic disorder alone reduces the exciton diffusion length more than one order of magnitude, from values typically encountered in molecules (> 50nm) to values actually measured in CPs (<10nm). 2) A number of organic crystals show anisotropic excitonic couplings, with weak interlayer interactions between molecules that are more strongly coupled within the layers. The resulting energy carriers are intra-layer 2D excitons that diffuse along the interlayer direction. We model this analytically for infinite layers and using quantum-chemical calculations of the electronic couplings for anthracene clusters. We show that the exciton hopping rates and diffusion lengths depend in a subtle manner on the size and shape of the interacting aggregates, temperature and the presence of energetic disorder. 3) The electronic structure at organic/organic interfaces plays a key role, among others, in defining the quantum efficiency of organic-based photovoltaic cells. Here, we perform quantum-chemical and microelectrostatic calculations on molecular aggregates of various sizes and shapes to characterize the interfacial dipole moment at pentacene/C60 heterojunctions. The results show that the interfacial dipole mostly originates in polarization effects due to the asymmetry in the multipolar expansion of the electronic density distribution between the interacting molecules. We will discuss how the quadrupoles on the pentacene molecules produce direct electrostatic interactions with charge carriers and how
Neither Goodenough ionic model nor Zener polaron model for Bi 0.5Ca 0.5Mn 1- xNi xO 3- δ system
NASA Astrophysics Data System (ADS)
Toulemonde, O.; Skovsen, I.; Mesguich, F.; Gaudin, E.
2008-04-01
The magnetic susceptibilities of three Bi 0.5Ca 0.5MnO 3- δ compounds synthesised by three different methods were characterised and analysed. Large magnetic Mn x clusters ( x ≥ 4) were considered to explain the high value of the Curie-Weiss constant. Unlike previous studies on similar systems, Goodenough ionic model or Zener polaron model is not suitable. In all cases, cluster behaviour is observed at low field and at low temperature. The influence of the oxygen stoichiometry and the homogeneity of the cation distribution depending on the method of the synthesis used is discussed. Finally, the effects of nickel doping on the magnetic properties were studied and the cluster behaviour was confirmed. The distribution in size of the clusters depends on the amount of nickel and it induces a glassy magnetic behaviour.
Exciton fine structure and spin relaxation in semiconductor colloidal quantum dots.
Kim, Jeongho; Wong, Cathy Y; Scholes, Gregory D
2009-08-18
semiconductors, fast energy relaxation among the QD exciton fine structure states is selectively measured. The measured exciton fine structure relaxation, which is a nanoscale analogue of molecular radiationless transitions, contains direct information on the relaxation of spin densities of electron and hole carriers, that is, spin relaxation in QDs. From the exciton fine structure relaxation rates measured for CdSe nanorods and complex-shaped nanocrystals using nonlinear polarization spectroscopy, we elucidated the implications of QD size and shape on the QD exciton properties as well, for example, size- and shape-scaling laws governing exciton spin flips and how an exciton is delocalized in a QD. We envision that the experimental development and the discoveries of QD exciton properties presented in this Account will inspire further studies toward revealing the characteristics of QD excitons and spin relaxation therein, for example, spin relaxation in QDs made of various materials with different electronic structures, spin relaxation under an external perturbation of QD electronic states using magnetic fields, and spin relaxation of separated electrons and holes in type-II QD heterostructures.
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
Selig, Malte; Berghäuser, Gunnar; Raja, Archana; ...
2016-11-07
Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetimemore » is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS2.« less
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
Selig, Malte; Berghäuser, Gunnar; Raja, Archana; Nagler, Philipp; Schüller, Christian; Heinz, Tony F.; Korn, Tobias; Chernikov, Alexey; Malic, Ermin; Knorr, Andreas
2016-11-07
Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. We investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS_{2} and MoSe_{2}) through a study combining microscopic theory with spectroscopic measurements. We also show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. Particularly, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures, in WS_{2}.
Excitonic linewidth and coherence lifetime in monolayer transition metal dichalcogenides
Selig, Malte; Berghäuser, Gunnar; Raja, Archana; Nagler, Philipp; Schüller, Christian; Heinz, Tony F.; Korn, Tobias; Chernikov, Alexey; Malic, Ermin; Knorr, Andreas
2016-01-01
Atomically thin transition metal dichalcogenides are direct-gap semiconductors with strong light–matter and Coulomb interactions. The latter accounts for tightly bound excitons, which dominate their optical properties. Besides the optically accessible bright excitons, these systems exhibit a variety of dark excitonic states. They are not visible in the optical spectra, but can strongly influence the coherence lifetime and the linewidth of the emission from bright exciton states. Here, we investigate the microscopic origin of the excitonic coherence lifetime in two representative materials (WS2 and MoSe2) through a study combining microscopic theory with spectroscopic measurements. We show that the excitonic coherence lifetime is determined by phonon-induced intravalley scattering and intervalley scattering into dark excitonic states. In particular, in WS2, we identify exciton relaxation processes involving phonon emission into lower-lying dark states that are operative at all temperatures. PMID:27819288
NASA Astrophysics Data System (ADS)
Xue, Fei; Wu, Feng Cheng; MacDonald, Allan
BEC of excitons and polaritons have drawn attention in recent years because of the demonstration of their ability to host macroscopic quantum phenomena and because of their promise for applications. We study the case of a system containing two TMD monolayers that are separated and surrounded by h-BN. Under appropriate conditions this system is expected to support a spatially indirect thermal equilibrium exciton condensate. We combine a microscopic mean-field calculation and a weakly interacting boson model to explore the bilayer exciton condensates phase diagram. By varying the layer separation and exciton density, we find a phase transition occurs between states containing one and two condensate flavors. We also use a microscopic time-dependent mean-field theory to address condensate collective mode spectra and quantum fluctuations. Next we study the case of exciton-polariton formed by strong coupling between quantum well excitons and confined photon modes when the system is placed in a vertical microcavity. We build a microscopic mean-field theory starting from electrons and holes, and account for their coupling to coherent light field. We compare our model with the normal weakly interacting boson model that starts from weakly interacting excitons that are coupled to photons. This work was supported by the SRC and NIST under the Nanoelectronic Research Initiative (NRI) and SWAN, by the Welch Foundation under Grant No. F1473, and by the ARO Grant No. 26-3508-81.
Excitons in Time-Dependent Density-Functional Theory.
Ullrich, Carsten A; Yang, Zeng-hui
2016-01-01
This chapter gives an overview of the description of the optical and dielectric properties of bulk insulators and semiconductors in time-dependent density-functional theory (TDDFT), with an emphasis on excitons. We review the linear-response formalism for periodic solids, discuss excitonic exchange-correlation kernels, calculate exciton binding energies for various materials, and compare the treatment of excitons with TDDFT and with the Bethe-Salpeter equation.
Probing Bose-Einstein condensation of excitons with electromagnetic radiation.
Johnsen, K; Kavoulakis, G M
2001-01-29
We examine the absorption spectrum of electromagnetic radiation from excitons, where an exciton in the 1s state absorbs a photon and makes a transition to the 2p state. We demonstrate that the absorption spectrum depends strongly on the quantum degeneracy of the exciton gas, and that it will generally manifest many-body effects. Based on our results we propose that absorption of infrared radiation could resolve recent contradictory experimental results on excitons in Cu(2)O.
Influence of excitonic effects on luminescence quantum yield in silicon
NASA Astrophysics Data System (ADS)
Sachenko, A. V.; Kostylyov, V. P.; Vlasiuk, V. M.; Sokolovskyi, I. O.; Evstigneev, M.
2017-03-01
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.
Excitonic interaction in the fluorene dimer
NASA Astrophysics Data System (ADS)
Wessel, John; Beck, Steven; Highstrete, Clark
1994-12-01
The fluorene van der Waals dimer exhibits a complex origin spectrum. This region has been studied by resonance two-photon ionization and by fluorescence excitation spectroscopies. The spectra can be interpreted on the basis of intermediate strength exciton coupling, in which the electronic interaction is comparable to the van der Waals vibrational energies. The spectra are reasonably well described by two distorted adiabatic potential surfaces, which correspond to the two excitonic components of the origin system. A single Franck-Condon active intermolecular mode provides a reasonable description of the system, however the potentials have significant cubic and quartic contributions. Non-Born-Oppenheimer nuclear momentum coupling is present and intermodal (IVR) interactions are observed, even for intermolecular modes as low as v=1. The results are remarkably different from prior observations of excitonic structure in other systems, providing a detailed picture of coupling between electronic and intermolecular motion in a van der Waals dimer.
Strong charge-transfer excitonic effects and the Bose-Einstein exciton condensate in graphane.
Cudazzo, Pierluigi; Attaccalite, Claudio; Tokatly, Ilya V; Rubio, Angel
2010-06-04
Using first principles many-body theory methods (GW+Bethe-Salpeter equation) we demonstrate that the optical properties of graphane are dominated by localized charge-transfer excitations governed by enhanced electron correlations in a two-dimensional dielectric medium. Strong electron-hole interaction leads to the appearance of small radius bound excitons with spatially separated electron and hole, which are localized out of plane and in plane, respectively. The presence of such bound excitons opens the path towards an excitonic Bose-Einstein condensate in graphane that can be observed experimentally.
PREFACE: International Conference on Optics of Excitons in Confined Systems
NASA Astrophysics Data System (ADS)
Viña, Luis; Tejedor, Carlos; Calleja, José M.
2010-01-01
The OECS11 (International Conference on Optics of Excitons in Confined Systems) was the eleventh of a very successful series of conferences that started in 1987 in Rome (Italy). Afterwards the conference was held at Naxos (Sicily, Italy, 1991), Montpellier (France, 1993), Cortona (Italy, 1995), Göttingen (Germany, 1997), Ascona (Switzerland, 1999), Montpellier (France, 2001), Lecce (Italy, 2003), Southampton (UK, 2005) and Patti (Sicily, Italy, 2007). It is addressed to scientists who lead fundamental and applied research on the optical properties of excitons in novel condensed-matter nanostructures. The 2009 meeting (7-11 September 2009) has brought together a large representation of the world leading actors in this domain, with the aim of stimulating the exchange of ideas, promoting international collaborations, and coordinating research on the newest exciton-related issues such as quantum information science and exciton quantum-collective phenomena. The meeting has included invited lectures, contributed oral presentations and posters, covering the following general topics: low-dimensional heterostructures: quantum wells, quantum wires and quantum dots polaritons quantum optics with excitons and polaritons many-body effects under coherent and incoherent excitation coherent optical spectroscopy quantum coherence and quantum-phase manipulation Bose-Einstein condensation and other collective phenomena excitons in novel materials The OECS 11 was held at the campus of the Universidad Autónoma de Madrid in Cantoblanco. The scientific program was composed of more than 200 contributions divided into 16 invited talks, 44 oral contributions and 3 poster sessions with a total of 150 presentations. The scientific level of the presentations was guaranteed by a selection process where each contribution was rated by three members of the Program Committee. The Conference has gathered 238 participants from 21 different countries, with the following distribution: Germany (43
Exciton dynamics in perturbed vibronic molecular aggregates
Brüning, C.; Wehner, J.; Hausner, J.; Wenzel, M.; Engel, V.
2015-01-01
A site specific perturbation of a photo-excited molecular aggregate can lead to a localization of excitonic energy. We investigate this localization dynamics for laser-prepared excited states. Changing the parameters of the electric field significantly influences the exciton localization which offers the possibility for a selective control of this process. This is demonstrated for aggregates possessing a single vibrational degree of freedom per monomer unit. It is shown that the effects identified for the molecular dimer can be generalized to larger aggregates with a high density of vibronic states. PMID:26798840
Tuneable paramagnetic susceptibility and exciton g-factor in Mn-doped PbS colloidal nanocrystals
NASA Astrophysics Data System (ADS)
Turyanska, L.; Hill, R. J. A.; Makarovsky, O.; Moro, F.; Knott, A. N.; Larkin, O. J.; Patanè, A.; Meaney, A.; Christianen, P. C. M.; Fay, M. W.; Curry, R. J.
2014-07-01
We report on PbS colloidal nanocrystals that combine within one structure solubility in physiological solvents with near-infrared photoluminescence, and magnetic and optical properties tuneable by the controlled incorporation of magnetic impurities (Mn). We use high magnetic fields (B up to 30 T) to measure the magnetization of the nanocrystals in liquid and the strength of the sp-d exchange interaction between the exciton and the Mn-ions. With increasing Mn-content from 0.1% to 7%, the mass magnetic susceptibility increases at a rate of ~10-7 m3 kg-1 per Mn percentage; correspondingly, the exciton g-factor decreases from 0.47 to 0.10. The controlled modification of the paramagnetism, fluorescence and exciton g-factor of the nanocrystals is relevant to the implementation of these paramagnetic semiconductor nanocrystals in quantum technologies ranging from quantum information to magnetic resonance imaging.We report on PbS colloidal nanocrystals that combine within one structure solubility in physiological solvents with near-infrared photoluminescence, and magnetic and optical properties tuneable by the controlled incorporation of magnetic impurities (Mn). We use high magnetic fields (B up to 30 T) to measure the magnetization of the nanocrystals in liquid and the strength of the sp-d exchange interaction between the exciton and the Mn-ions. With increasing Mn-content from 0.1% to 7%, the mass magnetic susceptibility increases at a rate of ~10-7 m3 kg-1 per Mn percentage; correspondingly, the exciton g-factor decreases from 0.47 to 0.10. The controlled modification of the paramagnetism, fluorescence and exciton g-factor of the nanocrystals is relevant to the implementation of these paramagnetic semiconductor nanocrystals in quantum technologies ranging from quantum information to magnetic resonance imaging. Electronic supplementary information (ESI) available: Details of the experiments techniques and results are available for the following studies: Raman and PL
Light induced polaron formation in perovskite solar cell devices
NASA Astrophysics Data System (ADS)
Neukirch, Amanda; Nie, Wanyi; Blancon, Jean-Christophe; Appavoo, Kannatassen; Tsai, Hsinhan; Chhowalla, Manish; Alam, Muhammad; Sfeir, Matthew; Katan, Claudine; Even, Jacky; Crochet, Jared; Gupta, Gautum; Mohite, Aditya; Tretiak, Sergei
The need for a low-cost, clean, and abundant source of energy has generated large amounts of research in solution processed solar cell materials. The lead halide perovskite has rapidly developed as a serious candidate for the active layer of photovoltaic devices. The efficiencies of devices made with this material have increased from 3.5% to over 20% in around 5 years. Despite the remarkable progress associated with perovskite materials, there are still fundamental questions regarding their lack of photo-stability over prolonged solar irradiation that need to be addressed. Recent experiments on photo-degradation under constant illumination have found fast self-healing by resting the device in the dark for less than 1 minute. Density functional theory and symmetry analysis show that localized charge states couple to local structural lattice distortions and methyl ammonium quasistatic configurations. Once translational symmetry is lost, additional bonding configurations become symmetry allowed, triggering localized charges in the vicinity over time under constant illumination, thus seeding the formation of macroscopic charged domains and preventing efficient charge extraction. Here we present an in-depth study of polaron formation and binding energy at the atomistic level.
Fragility, Intermediate Phase and Polaronic conductivity in heavy metal oxides
NASA Astrophysics Data System (ADS)
Chakraborty, Shibalik; Gunasekera, Kapila; Boolchand, Punit; Malki, Mohammed; Micoulaut, Matthieu
2013-03-01
The (B2O3)5 (TeO2)95-x (V2O5)x ternary forms bulk glasses over a wide range of compositions, 18% < x < 35%. Complex Cp(x) measurements as a function of modulation frequency reveal that melt fragility (m) show a global minimum (m = 52(2)) in the 23% < x < 26% range with m > 65 outside that window. These results suggest more stable network structure in the window than outside it. The fragility window coincides with a global minimum of the non-reversing enthalpy of relaxation at Tg, the reversibility window (23% < x < 27%), a behavior also found in chalcogenide glasses. Conductivity (σ) data show three regimes of variation; a low σ at x < 23%, a plateau in 23% < x < 27%, and an exponential increase at x > 27%. The reduced activation energy for conductivity at x > 27% is consistent with increased polaronic mobility as the network becomes flexible. These findings show glasses at x < 23% are stressed-rigid, in 23% < x < 27% range in the Intermediate Phase, and at x > 27% to be flexible. Supported by NSF grant DMR 08-53957.
Liquid-state polaron theory of the hydrated electron revisited
NASA Astrophysics Data System (ADS)
Donley, James P.; Heine, David R.; Tormey, Caleb A.; Wu, David T.
2014-07-01
The quantum path integral/classical liquid-state theory of Chandler and co-workers, created to describe an excess electron in solvent, is re-examined for the hydrated electron. The portion that models electron-water density correlations is replaced by two equations: the range optimized random phase approximation (RO-RPA), and the Donley, Rajasekaran, and Liu (DRL) approximation to the "two-chain" equation, both shown previously to describe accurately the static structure and thermodynamics of strongly charged polyelectrolyte solutions. The static equilibrium properties of the hydrated electron are analyzed using five different electron-water pseudopotentials. The theory is then compared with data from mixed quantum/classical Monte Carlo and molecular dynamics simulations using these same pseudopotentials. It is found that the predictions of the RO-RPA and DRL-based polaron theories are similar and improve upon previous theory, with values for almost all properties analyzed in reasonable quantitative agreement with the available simulation data. Also, it is found using the Larsen, Glover, and Schwartz pseudopotential that the theories give values for the solvation free energy that are at least three times larger than that from experiment.
Liquid-state polaron theory of the hydrated electron revisited
Donley, James P.; Heine, David R.; Tormey, Caleb A.; Wu, David T.
2014-07-14
The quantum path integral/classical liquid-state theory of Chandler and co-workers, created to describe an excess electron in solvent, is re-examined for the hydrated electron. The portion that models electron-water density correlations is replaced by two equations: the range optimized random phase approximation (RO-RPA), and the Donley, Rajasekaran, and Liu (DRL) approximation to the “two-chain” equation, both shown previously to describe accurately the static structure and thermodynamics of strongly charged polyelectrolyte solutions. The static equilibrium properties of the hydrated electron are analyzed using five different electron-water pseudopotentials. The theory is then compared with data from mixed quantum/classical Monte Carlo and molecular dynamics simulations using these same pseudopotentials. It is found that the predictions of the RO-RPA and DRL-based polaron theories are similar and improve upon previous theory, with values for almost all properties analyzed in reasonable quantitative agreement with the available simulation data. Also, it is found using the Larsen, Glover, and Schwartz pseudopotential that the theories give values for the solvation free energy that are at least three times larger than that from experiment.
Thermodynamics of the polaron master equation at finite bias
Krause, Thilo Brandes, Tobias; Schaller, Gernot; Esposito, Massimiliano
2015-04-07
We study coherent transport through a double quantum dot. Its two electronic leads induce electronic matter and energy transport and a phonon reservoir contributes further energy exchanges. By treating the system-lead couplings perturbatively, whereas the coupling to vibrations is treated non-perturbatively in a polaron-transformed frame, we derive a thermodynamic consistent low-dimensional master equation. When the number of phonon modes is finite, a Markovian description is only possible when these couple symmetrically to both quantum dots. For a continuum of phonon modes however, also asymmetric couplings can be described with a Markovian master equation. We compute the electronic current and dephasing rate. The electronic current enables transport spectroscopy of the phonon frequency and displays signatures of Franck-Condon blockade. For infinite external bias but finite tunneling bandwidths, we find oscillations in the current as a function of the internal bias due to the electron-phonon coupling. Furthermore, we derive the full fluctuation theorem and show its identity to the entropy production in the system.
Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla
Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T.; ...
2016-02-09
In bulk and quantum-confined semiconductors, magneto-optical studies have historically played an essential role in determining the fundamental parameters of excitons (size, binding energy, spin, dimensionality and so on). Here we report low-temperature polarized reflection spectroscopy of atomically thin WS2 and MoS2 in high magnetic fields to 65 T. Both the A and B excitons exhibit similar Zeeman splittings of approximately –230 μeV T–1 (g-factor ≃–4), thereby quantifying the valley Zeeman effect in monolayer transition-metal disulphides. Crucially, these large fields also allow observation of the small quadratic diamagnetic shifts of both A and B excitons in monolayer WS2, from which radiimore » of ~1.53 and ~1.16 nm are calculated. Further, when analysed within a model of non-local dielectric screening, these diamagnetic shifts also constrain estimates of the A and B exciton binding energies (410 and 470 meV, respectively, using a reduced A exciton mass of 0.16 times the free electron mass). Lastly, these results highlight the utility of high magnetic fields for understanding new two-dimensional materials.« less
Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla
NASA Astrophysics Data System (ADS)
Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T.; Kono, Junichiro; Crooker, Scott A.
2016-02-01
In bulk and quantum-confined semiconductors, magneto-optical studies have historically played an essential role in determining the fundamental parameters of excitons (size, binding energy, spin, dimensionality and so on). Here we report low-temperature polarized reflection spectroscopy of atomically thin WS2 and MoS2 in high magnetic fields to 65 T. Both the A and B excitons exhibit similar Zeeman splittings of approximately -230 μeV T-1 (g-factor ~=-4), thereby quantifying the valley Zeeman effect in monolayer transition-metal disulphides. Crucially, these large fields also allow observation of the small quadratic diamagnetic shifts of both A and B excitons in monolayer WS2, from which radii of ~1.53 and ~1.16 nm are calculated. Further, when analysed within a model of non-local dielectric screening, these diamagnetic shifts also constrain estimates of the A and B exciton binding energies (410 and 470 meV, respectively, using a reduced A exciton mass of 0.16 times the free electron mass). These results highlight the utility of high magnetic fields for understanding new two-dimensional materials.
Optically Detected Magnetic Resonance Studies on π-conjugated semiconductor systems
Chen, Ying
2011-01-01
Optically Detected Magnetic Resonance (ODMR) techniques were used to investigate the dynamics of excitons and charge carriers in π-conjugated organic semiconductors. Degradation behavior of the negative spin-1/2 electroluminescence-detected magnetic resonance (ELDMR) was observed in Alq3 devices. The increase in the resonance amplitude implies an increasing bipolaron formation during degradation, which might be the result of growth of charge traps in the device. The same behavior of the negative spin-1/2 ELDMR was observed in 2wt% Rubrene doped Tris(8-hydroxyquinolinato)aluminium (Alq3) devices. However, with increasing injection current, a positive spin-1/2 ELDMR, together with positive spin 1 triplet powder patterns at Δm_{S}=±1 and Δm_{S}=±2, emerges. Due to the similarities in the frequency dependences of single and double modulated ELDMR and the photoluminescence-detected magnetic resonance (PLDMR) results in poly[2-methoxy-5-(2 -ethyl-hexyloxy)-1,4-phenyl ene vinylene] (MEH-PPV) films, the mechanism for this positive spin-1/2 ELDMR was assigned to enhanced triplet-polaron quenching under resonance conditions. The ELDMR in rubrene doped Alq3 devices provides a path to investigate charge distribution in the device under operational conditions. Combining the results of several devices with different carrier blocking properties and the results from transient EL, it was concluded trions not only exist near buffer layer but also exist in the electron transport layer. This TPQ model can also be used to explain the positive spin-1/2 PLDMR in poly(3-hexylthiophene) (P3HT) films at low temperature and in MEH-PPV films at various temperatures up to room temperature. Through quantitative analysis, TE-polaron quenching (TPQ) model is shown having the ability to explain most behaviors of the positive spin-1/2 resonance. Photocurrent detected magnetic resonance (PCDMR) studies on MEH-PPV devices revealed a novel transient resonance signal. The signal
Bright and dark excitons in semiconductor carbon nanotubes
Tretiak, Sergei
2008-01-01
We report electronic structure calculations of finite-length semiconducting carbon nanotubes using the time dependent density functional theory (TD-DFT) and the time dependent Hartree Fock (TD-HF) approach coupled with semiempirical AM1 and ZINDO Hamiltonians. We specifically focus on the energy splitting, relative ordering, and localization properties of the optically active (bright) and optically forbidden (dark) states from the lowest excitonic band of the nanotubes. These excitonic states are very important in competing radiative and non-radiative processes in these systems. Our analysis of excitonic transition density matrices demonstrates that pure DFT functionals overdelocalize excitons making an electron-hole pair unbound; consequently, excitonic features are not presented in this method. In contrast, the pure HF and A111 calculations overbind excitons inaccurately predicting the lowest energy state as a bright exciton. Changing AM1 with ZINDO Hamiltonian in TD-HF calculations, predicts the bright exciton as the second state after the dark one. However, in contrast to AM1 calculations, the diameter dependence of the excitation energies obtained by ZINDO does not follow the experimental trends. Finally, the TD-DFT approach incorporating hybrid functions with a moderate portion of the long-range HF exchange, such as B3LYP, has the most generality and predictive capacity providing a sufficiently accurate description of excitonic structure in finite-size nanotubes. These methods characterize four important lower exciton bands. The lowest state is dark, the upper band is bright, and the two other dark and nearly degenerate excitons lie in-between. Although the calculated energy splittings between the lowest dark and the bright excitons are relatively large ({approx}0.1 eV), the dense excitonic manifold below the bright exciton allows for fast non-radiative relaxation leasing to the fast population of the lowest dark exciton. This rationalizes the low
All-coupling polaron optical response: Analytic approaches beyond the adiabatic approximation
NASA Astrophysics Data System (ADS)
Klimin, S. N.; Tempere, J.; Devreese, J. T.
2016-09-01
In the present work, the problem of an all-coupling analytic description for the optical conductivity of the Fröhlich polaron is treated, with the goal being to bridge the gap in the validity range that exists between two complementary methods: on the one hand, the memory-function formalism and, on the other hand, the strong-coupling expansion based on the Franck-Condon picture for the polaron response. At intermediate coupling, both methods were found to fail as they do not reproduce diagrammatic quantum Monte Carlo results. To resolve this, we modify the memory-function formalism with respect to the Feynman-Hellwarth-Iddings-Platzman approach in order to take into account a nonquadratic interaction in a model system for the polaron. The strong-coupling expansion is extended beyond the adiabatic approximation by including in the treatment nonadiabatic transitions between excited polaron states. The polaron optical conductivity that we obtain at T =0 by combining the two extended methods agrees well, both qualitatively and quantitatively, with the diagrammatic quantum Monte Carlo results in the whole available range of the electron-phonon coupling strength.
First-principles study of hole polaron formation and migration in SrI2
NASA Astrophysics Data System (ADS)
Zhou, Fei; Sadigh, Babak; Aberg, Daniel
2015-03-01
We investigate the formation of self-trapped holes (STH) in the high performance scintillator material SrI2 using a recently developed first principles method, polaron self-interaction correction (pSIC). pSIC removes the significant spurious self-interaction of localized polaron states. It is capable of accurately reproduce the configurational energy landscape of polaronic states from optimized hybrid functionals at the computational cost of the local density approximation. We searched for and identified all symmetrically distinct STH states localized on neighboring I-I dimers, i.e. Vk centers, and found non-trivial relation between the STH formation energies and dimer separation. All possible polaron hopping paths of the type IAIB -->IBIC are investigated systematically with pSIC and the elastic band method, and paths with low migration barrier energy of about 0.2 eV were identified, suggesting high mobility in SrI2. We expect that the present approach can be applied to study polaron formation and migration in other materials. Support from the National Nuclear Security Administration Office of Nonproliferation Research and Development (NA-22) is acknowledged. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore N We acknowledge funding from the NA-22 agency.
Small polaron hopping conduction mechanism in LiFePO4 glass and crystal
NASA Astrophysics Data System (ADS)
Banday, Azeem; Murugavel, Sevi
2017-01-01
The optimization of a cathode material is the most important criterion of lithium ion battery technology, which decides the power density. In order to improve the rate capability, a cathode material must possess high electronic and ionic conductivities. Therefore, it is important to understand the charge transport mechanism in such an advanced cathode material in its intrinsic state before modifying it by various means. In this work, we report the thermal, structural, and electrical conductivity studies on lithium iron phosphate, LiFePO4, both in its polycrystalline (LFPC) and glassy (LFPG) counterpart states. The vibrational spectroscopic measurements reveal the characteristic vibrational modes, which are the intrinsic part of LFPC, whereas in LFPG, the phonon modes become broader and overlap with each other due to the lattice disorder. The electrical conductivity measurements reveal that LFPG exhibits a higher polaronic conductivity of 1.6 orders than the LFPC sample. The temperature dependent dc conductivity has been analyzed with the Mott model of polarons and reveals the origin of enhanced polaronic conductivity in LFPG. Based on the analysis, the enhanced polaronic conductivity in LFPG has been attributed to the combined effect of reduced hopping length, decreased activation energy, and enhanced polaron concentration.
Tunable Polarons of Slow-Light Polaritons in a Two-Dimensional Bose-Einstein Condensate
NASA Astrophysics Data System (ADS)
Grusdt, Fabian; Fleischhauer, Michael
2016-02-01
When an impurity interacts with a bath of phonons it forms a polaron. For increasing interaction strengths the mass of the polaron increases and it can become self-trapped. For impurity atoms inside an atomic Bose-Einstein condensate (BEC) the nature of this transition is not understood. While Feynman's variational approach to the Fröhlich model predicts a sharp transition for light impurities, renormalization group studies always predict an extended intermediate-coupling region characterized by large phonon correlations. To investigate this intricate regime and to test polaron physics beyond the validity of the Fröhlich model we suggest a versatile experimental setup that allows us to tune both the mass of the impurity and its interactions with the BEC. The impurity is realized as a dark-state polariton (DSP) inside a quasi-two-dimensional BEC. We show that its interactions with the Bogoliubov phonons lead to photonic polarons, described by the Bogoliubov-Fröhlich Hamiltonian, and make theoretical predictions using an extension of a recently introduced renormalization group approach to Fröhlich polarons.
Free-exciton states in crystalline GaTe
NASA Astrophysics Data System (ADS)
Wan, J. Z.; Brebner, J. L.; Leonelli, R.
1995-12-01
Polarized properties of both the singlet and triplet ground exciton states in the photoluminescence and transmission spectra of crystalline GaTe are explained based on the possible symmetry properties of the energy band edge of GaTe. Some experimental results about excited exciton states in GaTe are presented and discussed. The energy positions of exciton series in GaTe follow the three-dimensional direct allowed Wannier exciton formula just as in the the other III-VI layered compounds of GaSe and InSe. The nonthermalized, ``hot'' nature of excitons inside GaTe under higher optical excitation intensities is also discussed.
Exciton dynamics in a single layer MoS2
NASA Astrophysics Data System (ADS)
Kim, Jonghwan; Hong, Xiaoping; Shi, Sufei; Jin, Chenhao; Sun, Yinghui; Wang, Feng
2014-03-01
In a low dimensional semiconductor, exciton plays a crucial role in the optical property. Recently, a single layer of MoS2 has attracted significant attention due to its unique excitonic features. For example, exciton in MoS2 is predicted to have order of magnitude larger binding energy than conventional direct band gap material. For deeper understanding on such properties, however, it is important to understand how exciton is formed and decays in time domain. Our work on exciton dynamics in MoS2 by pump probe spectroscopy will be presented with control of both power and wavelength.
(Gene sequencing by scanning molecular exciton microscopy)
Not Available
1991-01-01
This report details progress made in setting up a laboratory for optical microscopy of genes. The apparatus including a fluorescence microscope, a scanning optical microscope, various spectrometers, and supporting computers is described. Results in developing photon and exciton tips, and in preparing samples are presented. (GHH)
Multiple exciton generation in colloidal silicon nanocrystals.
Beard, Matthew C; Knutsen, Kelly P; Yu, Pingrong; Luther, Joseph M; Song, Qing; Metzger, Wyatt K; Ellingson, Randy J; Nozik, Arthur J
2007-08-01
Multiple exciton generation (MEG) is a process whereby multiple electron-hole pairs, or excitons, are produced upon absorption of a single photon in semiconductor nanocrystals (NCs) and represents a promising route to increased solar conversion efficiencies in single-junction photovoltaic cells. We report for the first time MEG yields in colloidal Si NCs using ultrafast transient absorption spectroscopy. We find the threshold photon energy for MEG in 9.5 nm diameter Si NCs (effective band gap identical with Eg = 1.20 eV) to be 2.4 +/- 0.1Eg and find an exciton-production quantum yield of 2.6 +/- 0.2 excitons per absorbed photon at 3.4Eg. While MEG has been previously reported in direct-gap semiconductor NCs of PbSe, PbS, PbTe, CdSe, and InAs, this represents the first report of MEG within indirect-gap semiconductor NCs. Furthermore, MEG is found in relatively large Si NCs (diameter equal to about twice the Bohr radius) such that the confinement energy is not large enough to produce a large blue-shift of the band gap (only 80 meV), but the Coulomb interaction is sufficiently enhanced to produce efficient MEG. Our findings are of particular importance because Si dominates the photovoltaic solar cell industry, presents no problems regarding abundance and accessibility within the Earth's crust, and poses no significant environmental problems regarding toxicity.
Revealing the nature of excitons in liquid exfoliated monolayer tungsten disulphide
NASA Astrophysics Data System (ADS)
Kłopotowski, Ł.; Backes, C.; Mitioglu, A. A.; Vega-Mayoral, V.; Hanlon, D.; Coleman, J. N.; Ivanov, V. Y.; Maude, D. K.; Plochocka, P.
2016-10-01
Transition metal dichalcogenides (TMD) hold promise for applications in novel optoelectronic devices. There is therefore a need for materials that can be obtained in large quantities and with well understood optical properties. In this report, we present thorough photoluminescence (PL) investigations of monolayer tungsten disulphide obtained via liquid phase exfoliation. As shown by microscopy studies, the exfoliated nanosheets have dimensions of tens of nanometers and thickness of 2.5 monolayers on average. The monolayer content is about 20%. Our studies show that at low temperature the PL is dominated by excitons localized on nanosheet edges. As a consequence, the PL is strongly sensitive to the environment and exhibits an enhanced splitting in magnetic field. As the temperature is increased, the excitons are thermally excited out of the defect states and the dominant transition is that of the negatively charged exciton. Furthermore, upon excitation with a circularly polarized light, the PL retains a degree of polarization reaching 50% and inherited from the valley polarized photoexcited excitons. The studies of PL dynamics reveal that the PL lifetime is on the order of 10 ps, which is probably limited by non-radiative processes. Our results underline the potential of liquid exfoliated TMD monolayers in large scale optoelectronic devices.
Morphology effects of self-assembled quantum dots on the energy spectrum of magneto-excitons
NASA Astrophysics Data System (ADS)
Villamil, Pablo; Sierra Ortega, José
2014-02-01
In this paper we analyze the changes experienced by the energy spectra of a confined exciton in type II semiconductor quantum dots, considering the quantum dot as a possible functional part that, in the future devices, can be applied in spintronics, optoelectronics, and quantum information technologies. We studied the lowest energy states of an exciton (X) confined in type II InP/GaInP self-assembled quantum dot (SAQDs), with axial symmetry in the presence of a uniformly applied magnetic field in the growth direction. In our model, it is considered that the electron is located within the point of InP and the hole is in the GaInP barrier. The solution of the Schrödinger equation for this system is obtained by a variational separation process of variables in the adiabatic approximation limit and within the effective mass approximation. We study the energy levels associated with the electron and the hole, and the energy of the exciton. Due to the axial symmetry of the problem the z component of the total orbital angular momentum, Lz=le+lh, is preserved and the exciton states are classified according to the values of this component. Quantum dots have a finite and variable thickness, with the purpose of analyzing the effects related to the variation of the morphology and the presence of a wet layer.
Light-hole exciton in a nanowire quantum dot
NASA Astrophysics Data System (ADS)
Jeannin, Mathieu; Artioli, Alberto; Rueda-Fonseca, Pamela; Bellet-Amalric, Edith; Kheng, Kuntheak; André, Régis; Tatarenko, Serge; Cibert, Joël; Ferrand, David; Nogues, Gilles
2017-01-01
Quantum dots inserted inside semiconductor nanowires are extremely promising candidates as building blocks for solid-state-based quantum computation and communication. They provide very high crystalline and optical properties and offer a convenient geometry for electrical contacting. Having a complete determination and full control of their emission properties is one of the key goals of nanoscience researchers. Here we use strain as a tool to create in a single magnetic nanowire quantum dot a light-hole exciton, an optically active quasiparticle formed from a single electron bound to a single light hole. In this frame, we provide a general description of the mixing within the hole quadruplet induced by strain or confinement. A multi-instrumental combination of cathodoluminescence, polarization-resolved Fourier imaging, and magneto-optical spectroscopy, allows us to fully characterize the hole ground state, including its valence band mixing with heavy-hole states.
Warping and interactions of vortices in exciton-polariton condensates
NASA Astrophysics Data System (ADS)
Toledo-Solano, M.; Mora-Ramos, M. E.; Figueroa, A.; Rubo, Y. G.
2014-01-01
We investigate the properties of the vortex singularities in two-component exciton-polariton condensates in semiconductor microcavities in the presence of transverse-electric-transverse-magnetic (TE-TM) splitting of the lower polariton branch. This splitting does not change qualitatively the basic (lemon and star) geometry of half-quantum vortices (HQVs), but results in warping of both the polarization field and the supercurrent streamlines around these entities. The TE-TM splitting has a pronounced effect on the HQV energies and interactions, as well as on the properties of integer vortices, especially on the energy of the hedgehog polarization vortex. The energy of this vortex can become smaller than the energies of HQVs. This leads to modification of the Berezinskii-Kosterlitz-Thouless transition from the proliferation of half-vortices to the proliferation of hedgehog-based vortex molecules.
Spin-triplet negatively charged excitons in GaAs quantum wells
NASA Astrophysics Data System (ADS)
Shields, A. J.; Pepper, M.; Simmons, M. Y.; Ritchie, D. A.
1995-09-01
We observe magnetic-field-induced transitions in the interband optical spectra of GaAs quantum wells with a small excess electron density. Their strengthening with excess electron density, in addition to their light polarization dependence, demonstrate that these correspond to (excited) spin-triplet states of the negatively charged exciton. The second-electron binding energy of both singlet and triplet X- strengthens with field.
Exciton strings in an organic charge-transfer crystal
NASA Astrophysics Data System (ADS)
Kuwata-Gonokami, M.; Peyghambarian, N.; Meissner, K.; Fluegel, B.; Sato, Y.; Ema, K.; Shimano, R.; Mazumdar, S.; Guo, F.; Tokihiro, T.; Ezaki, H.; Hanamura, E.
1994-01-01
COLLECTIVE excitations resulting from many-body Coulomb interactions have been studied extensively in the solid state1: for example, the exchange interaction between the electrons in two excitons (bound electron-hole pairs) can bind the excitons together, forming a biexciton. At the other extreme, if the number of excitons is sufficiently large (~106), they can condense into a degenerate 'liquid' phase known as an electron-hole drop. But in conventional semiconductors, intermediate bound states, consisting of more than two excitons, are not formed. We show here, both theoretically and experimentally, that bound states of multiple excitons can form in the organic charge-transfer solid anthracene-(pyromellitic acid dianhydride). Coulomb interactions along the one-dimensional stacks of this material can stabilize trains of several charge-transfer excitons, and we refer to the resulting collective excitations as exciton strings.
Coupled exciton-photon Bose condensate in path integral formalism
NASA Astrophysics Data System (ADS)
Elistratov, A. A.; Lozovik, Yu. E.
2016-03-01
We study the behavior of exciton polaritons in an optical microcavity with an embedded semiconductor quantum well. We use a two-component exciton-photon approach formulated in terms of path integral formalism. In order to describe spatial distributions of the exciton and photon condensate densities, the two coupled equations of the Gross-Pitaevskii type are derived. For a homogeneous system, we find the noncondensate photon and exciton spectra, calculate the coefficients of transformation from the exciton-photon basis to the lower-upper polariton basis, and obtain the exciton and photon occupation numbers of the lower and upper polariton branches for nonzero temperatures. For an inhomogeneous system, the set of coupled equations of the Bogoliubov-de Gennes type is derived. The equations govern the spectra and spatial distributions of noncondensate photons and excitons.
Eersel, H. van Coehoorn, R.; Bobbert, P. A.; Janssen, R. A. J.
2014-10-06
We present an advanced molecular-scale organic light-emitting diode (OLED) model, integrating both electronic and excitonic processes. Using this model, we can reproduce the measured efficiency roll-off for prototypical phosphorescent OLED stacks based on the green dye tris[2-phenylpyridine]iridium (Ir(ppy){sub 3}) and the red dye octaethylporphine platinum (PtOEP) and study the cause of the roll-off as function of the current density. Both the voltage versus current density characteristics and roll-off agree well with experimental data. Surprisingly, the results of the simulations lead us to conclude that, contrary to what is often assumed, not triplet-triplet annihilation but triplet-polaron quenching is the dominant mechanism causing the roll-off under realistic operating conditions. Simulations for devices with an optimized recombination profile, achieved by carefully tuning the dye trap depth, show that it will be possible to fabricate OLEDs with a drastically reduced roll-off. It is envisaged that J{sub 90}, the current density at which the efficiency is reduced to 90%, can be increased by almost one order of magnitude as compared to the experimental state-of-the-art.
NASA Astrophysics Data System (ADS)
Kalosakas, G.; Aubry, S.; Tsironis, G. P.
1998-10-01
We use a stationary and normal mode analysis of the semiclassical Holstein model in order to connect the low-frequency linear polaron modes to low-lying far-infrared lines of the acetanilide spectrum and through parameter fitting we comment on the validity of the polaron results in this system.
Characterization of Macroscopic Ordering in Exciton Rings
NASA Astrophysics Data System (ADS)
Yang, Sen; Levitov, L. S.; Simons, B. D.; Gossard, A. C.
2005-03-01
Recently observed complex PL patterns in 2D QW structures exhibit the inner [1,3] and the outer [1-4] exciton rings, localized bright spots [1,3], and the macroscopically ordered exciton state (MOES) [1,3]. The latter appears at the outer ring via its fragmentation into a periodic array of aggregates. While the gross features have been explained within classical framework, attributing the inner rings to nonradiative exciton transport and cooling [1], and the outermost rings and the bright spots to macroscopic charge separation [3,4], the origin of the MOES remains unidentified [5]. Here, for the first time, we report experiments demonstrating the exciton energy modulation over the MOES as well as the phase diagram of MOES in exciton density and temperature coordinates. The experiments shed new light on the dynamical origin of MOES. Besides, we present the studies of dynamical processes within MOES including the observation of aggregate instabilities and bifurcations that point to the spontaneous character of the instability.[1] L.V. Butov, A.C. Gossard, D.S. Chemla, Nature 418, 751 (2002). [2] D. Snoke, S. Denev, Y. Liu, L. Pfeiffer, K. West, Nature 418, 754 (2002). [3] L.V. Butov, L.S. Levitov, A.V. Mintsev, B.D. Simons, A.C. Gossard, D.S. Chemla PRL 92, 117404 (2004). [4] R. Rapaport, G. Chen, D. Snoke, S.H. Simon, L. Pfeiffer, K. West, Y. Liu, S. Denev PRL 92, 117405 (2004). [5] L.S. Levitov, B.D. Simons, L.V. Butov, cond-mat/0403377.
Zhou, Fei; Sadigh, Babak; Aberg, Daniel; ...
2016-08-12
The excellent light yield proportionality of europium-doped strontium iodide (SrI2:Eu) has resulted in state-of-the-art γ-ray detectors with remarkably high-energy resolution, far exceeding that of most halide compounds. In this class of materials, the formation of self-trapped hole polarons is very common. However, polaron formation is usually expected to limit carrier mobilities and has been associated with poor scintillator light-yield proportionality and resolution. Here using a recently developed first-principles method, we perform an unprecedented study of polaron transport in SrI2, both for equilibrium polarons, as well as nascent polarons immediately following a self-trapping event. We propose a rationale for the unexpectedmore » high-energy resolution of SrI2. We identify nine stable hole polaron configurations, which consist of dimerised iodine pairs with polaron-binding energies of up to 0.5 eV. They are connected by a complex potential energy landscape that comprises 66 unique nearest-neighbour migration paths. Ab initio molecular dynamics simulations reveal that a large fraction of polarons is born into configurations that migrate practically barrier free at room temperature. Consequently, carriers created during γ-irradiation can quickly diffuse away reducing the chance for nonlinear recombination, the primary culprit for non-proportionality and resolution reduction. We conclude that the flat, albeit complex, landscape for polaron migration in SrI2 is a key for understanding its outstanding performance. This insight provides important guidance not only for the future development of high-performance scintillators but also of other materials, for which large polaron mobilities are crucial such as batteries and solid-state ionic conductors.« less
Zhou, Fei; Sadigh, Babak; Aberg, Daniel; Erhart, Paul
2016-08-12
The excellent light yield proportionality of europium-doped strontium iodide (SrI_{2}:Eu) has resulted in state-of-the-art γ-ray detectors with remarkably high-energy resolution, far exceeding that of most halide compounds. In this class of materials, the formation of self-trapped hole polarons is very common. However, polaron formation is usually expected to limit carrier mobilities and has been associated with poor scintillator light-yield proportionality and resolution. Here using a recently developed first-principles method, we perform an unprecedented study of polaron transport in SrI_{2}, both for equilibrium polarons, as well as nascent polarons immediately following a self-trapping event. We propose a rationale for the unexpected high-energy resolution of SrI_{2}. We identify nine stable hole polaron configurations, which consist of dimerised iodine pairs with polaron-binding energies of up to 0.5 eV. They are connected by a complex potential energy landscape that comprises 66 unique nearest-neighbour migration paths. Ab initio molecular dynamics simulations reveal that a large fraction of polarons is born into configurations that migrate practically barrier free at room temperature. Consequently, carriers created during γ-irradiation can quickly diffuse away reducing the chance for nonlinear recombination, the primary culprit for non-proportionality and resolution reduction. We conclude that the flat, albeit complex, landscape for polaron migration in SrI_{2} is a key for understanding its outstanding performance. This insight provides important guidance not only for the future development of high-performance scintillators but also of other materials, for which large polaron mobilities are crucial such as batteries and solid-state ionic conductors.
Bloch oscillations as generators of polarons in a 1D crystal
NASA Astrophysics Data System (ADS)
Nazareno, H. N.; Brito, P. E. de
2016-08-01
The main purpose of this work is to characterize the kind of propagation/localization of carriers in a one-dimensional crystalline structure along the tight-binding model while the electron-phonon interaction is taken into account through a deformation potential and the system is under the action of a dc electric field. The lattice was treated in the classical formalism of harmonic vibrations. A remarkable effect is obtained due to the presence of the electric field. On one side the particle performs Bloch oscillations and at the same time it interacts with the lattice and as a result at each turning point of its trajectory phonons are generated that carry with them a fraction of the electronic wave packet, it is the polaron formation. This way the Bloch oscillations pump polarons into the system. We explain why the polaron is formed at returning points of the oscillations.
Dynamics of exciton transfer in coupled polymer chains
NASA Astrophysics Data System (ADS)
Zhang, Y. L.; Liu, X. J.; Sun, Z.; An, Z.
2013-05-01
The dynamics of singlet and triplet exciton transfer in coupled polymer chains are investigated within the Su-Schrieffer-Heeger+Pariser-Parr-Pople model including both electron-phonon (e-p) coupling and electron-electron (e-e) interactions, using a multi-configurational time-dependent Hartree-Fock dynamic method. In order to explain the processes involved, the effects of on-site and long-range e-e interactions on the locality of the singlet and triplet excitons are first investigated on an isolated chain. It is found that the locality of the singlet exciton decreases, while the locality of the triplet exciton increases with an increase in the on-site e-e interactions. On the other hand, an increase in the long-range e-e interaction results in a more localized singlet exciton and triplet exciton. In coupled polymer chains, we then quantitatively show the yields of singlet and triplet exciton transfer products under the same interchain coupling. It is found that the yield of singlet interchain excitons is much higher than that of triplet interchain excitons, that is to say, singlet exciton transfer is significantly easier than that for triplet excitons. This results from the fact that the singlet exciton is more delocalized than the triplet exciton. In addition, hopping of electrons with opposite spins between the coupled chains can facilitate the transfer of singlet excitons. The results are of great significance for understanding the photoelectric conversion process and developing high-power organic optoelectronic applications.
Polaronic approach to strongly correlated electron systems with strong electron-phonon interaction
NASA Astrophysics Data System (ADS)
Makarov, I. A.; Shneyder, E. I.; Kozlov, P. A.; Ovchinnikov, S. G.
2015-10-01
The three-band p -d model of strongly correlated electrons interacting with optical phonons via diagonal and off-diagonal electron-phonon interactions is considered within the cluster perturbation theory. In the beginning, the exact diagonalization of the Hamiltonian of a CuO4 cluster results in the construction of local polaronic eigenstates |p > with hole numbers nh=0 ,1 ,2 per unit cell. The intercluster hoppings and interactions are exactly written in terms of Hubbard operators Xfp q=|p >polaronic eigenstates |p > at site f . The Fermi-type single-electron quasiparticle dispersion and spectral weight are calculated for the undoped antiferromagnetic parent insulator like La2CuO4 . The quasiparticle dispersion of Hubbard polarons is determined by a hybridization of the Hubbard fermion subbands with local Franck-Condon resonances so the main polaronic effect of the quasiparticle band structure is a splitting of the Hubbard bands on the number of Hubbard polaron subbands. Increasing of the EPI constant results in an increase of splitting, decrease of the subband width, transfer of the spectral weight to high-energy multiphonon excitations, and subsequent localization of the charge carriers. Herewith, the effect of such renormalization for the conduction band and the valence one differs depending on the ratio of the diagonal and off-diagonal EPI. In the framework of the GTB method, the Franck-Condon broadening of the spectral function of polaronic excitations is also reproduced for strongly correlated systems with strong electron-phonon interaction.
Q1D-Polarons in Rigid Boundary Cylindrical Wires: "Mixed-Coupling Approximation"
NASA Astrophysics Data System (ADS)
Senger, R. T.; Erçelebý, A.
1998-02-01
We consider the interaction of a confined electron with bulk polar-optical phonons in a cylindrical quantum well wire with infinite boundary potential. Expressions for the polaron self energy and mass are derived within a composite variational scheme consisting of a strong-coupling characterization imposed in the lateral directions and a weak-coupling LLP-counterpart structured along the length of the wire. The formulation is seen to be rather commendable and yields a sensible description of the Q1D-polaron in thin wires of weak or intermediate electron-phonon coupling strengths.
Effects of Shannon entropy and electric field on polaron in RbCl triangular quantum dot
NASA Astrophysics Data System (ADS)
M, Tiotsop; A, J. Fotue; S, C. Kenfack; N, Issofa; H, Fotsin; L, C. Fai
2016-04-01
In this paper, the time evolution of the quantum mechanical state of a polaron is examined using the Pekar type variational method on the condition of the electric-LO-phonon strong-coupling and polar angle in RbCl triangular quantum dot. We obtain the eigenenergies, and the eigenfunctions of the ground state, and the first excited state respectively. This system in a quantum dot can be treated as a two-level quantum system qubit and the numerical calculations are performed. The effects of Shannon entropy and electric field on the polaron in the RbCl triangular quantum dot are also studied.
Zeković, Slobodan; Ivić, Zoran
2009-01-01
The applicability of small-polaron model for the interpretation of infrared absorption spectrum in acetanilide has been critically reexamined. It is shown that the energy difference between the normal and anomalous peak, calculated by means of small-polaron theory, displays pronounced temperature dependence which is in drastic contradiction with experiment. It is demonstrated that self-trapped states, which are recently suggested to explain theoretically the experimental absorption spectrum in protein, cannot cause the appearance of the peaks in absorption spectrum for acetanilide.
Evidence for Light-Induced Hole Polarons in LiNbO3
NASA Astrophysics Data System (ADS)
Herth, P.; Granzow, T.; Schaniel, D.; Woike, Th.; Imlau, M.; Krätzig, E.
2005-08-01
Transient light-induced absorption in LiNbO3 is observed in the blue-green spectral range after pulsed illumination with 532 nm. Its buildup and decay in Fe-doped LiNbO3 is satisfactorily described by a sum of two stretched exponential functions. For undoped LiNbO3, however, only one stretched exponential decay is observed. These experimental results are explained by the formation of both small Nb4+Li electron polarons and O- hole polarons. The mechanism is discussed on the basis of a proposed band scheme.
Polaron dynamics with off-diagonal coupling: beyond the Ehrenfest approximation.
Huang, Zhongkai; Wang, Lu; Wu, Changqin; Chen, Lipeng; Grossmann, Frank; Zhao, Yang
2017-01-04
Treated traditionally by the Ehrenfest approximation, the dynamics of a one-dimensional molecular crystal model with off-diagonal exciton-phonon coupling is investigated in this work using the Dirac-Frenkel time-dependent variational principle with the multi-D2Ansatz. It is shown that the Ehrenfest method is equivalent to our variational method with the single D2Ansatz, and with the multi-D2Ansatz, the accuracy of our simulated dynamics is significantly enhanced in comparison with the semi-classical Ehrenfest dynamics. The multi-D2Ansatz is able to capture numerically accurate exciton momentum probability and help clarify the relation between the exciton momentum redistribution and the exciton energy relaxation. The results demonstrate that the exciton momentum distributions in the steady state are determined by a combination of the transfer integral and the off-diagonal coupling strength, independent of the excitonic initial conditions. We also probe the effect of the transfer integral and the off-diagonal coupling on exciton transport in both real and reciprocal space representations. Finally, the variational method with importance sampling is employed to investigate temperature effects on exciton transport using the multi-D2Ansatz, and it is demonstrated that the variational approach is valid in both low and high temperature regimes.
Exciton radiative lifetime in transition metal dichalcogenide monolayers
NASA Astrophysics Data System (ADS)
Robert, C.; Lagarde, D.; Cadiz, F.; Wang, G.; Lassagne, B.; Amand, T.; Balocchi, A.; Renucci, P.; Tongay, S.; Urbaszek, B.; Marie, X.
2016-05-01
We have investigated the exciton dynamics in transition metal dichalcogenide monolayers using time-resolved photoluminescence experiments performed with optimized time resolution. For MoS e2 monolayer, we measure τrad0=1.8 ±0.2 ps at T =7 K that we interpret as the intrinsic radiative recombination time. Similar values are found for WS e2 monolayers. Our detailed analysis suggests the following scenario: at low temperature (T ≲50 K ), the exciton oscillator strength is so large that the entire light can be emitted before the time required for the establishment of a thermalized exciton distribution. For higher lattice temperatures, the photoluminescence dynamics is characterized by two regimes with very different characteristic times. First the photoluminescence intensity drops drastically with a decay time in the range of the picosecond driven by the escape of excitons from the radiative window due to exciton-phonon interactions. Following this first nonthermal regime, a thermalized exciton population is established gradually yielding longer photoluminescence decay times in the nanosecond range. Both the exciton effective radiative recombination and nonradiative recombination channels including exciton-exciton annihilation control the latter. Finally the temperature dependence of the measured exciton and trion dynamics indicates that the two populations are not in thermodynamical equilibrium.
A new class of collective excitations: Exciton strings
NASA Astrophysics Data System (ADS)
Mazumdar, S.; Guo, F.; Meissner, K.; Fluegel, B.; Peyghambarian, N.
1996-06-01
Optical excitation in a strongly neutral quasi-one-dimensional mixed-stack charge-transfer solid results in an exciton state, in which the electron and the hole are bound by electrostatic Coulomb interactions that are large compared to the one-electron hopping. We present a joint theoretical-experimental demonstration of a new class of collective excitations, multiexcitons or exciton strings, consisting of a string of several (more than two) bound excitons, in a prototype neutral charge-transfer solid. The stability of the multiexciton states arise from the combined effects of one dimensionality and strong Coulomb interactions. Theoretically, we show that in narrow band one-dimensional semiconductors with long range Coulomb interactions, the occurrence of stable 2-exciton string (biexciton) necessarily implies stable higher multiexcitons. Experimentally, evidence for the multiexciton strings is demonstrated by femtosecond pump-probe spectroscopy of anthracene pyromellitic acid dianhydride. Excellent qualitative agreement is found between the calculated and the measured differential transmission spectra. Photoinduced absorptions to the 2-exciton string at low pump intensity and to the 3-exciton string at high pump intensity are observed, in agreement with the theory of excited state absorption. The 2-exciton string is confirmed also by a direct two-photon absorption measurement. The binding energies of the 2-exciton and the 3-exciton strings are obtained from the experimental data. The larger binding energy of the 3-exciton is in agreement with theory.
Fine structure of the exciton electroabsorption in semiconductor superlattices
NASA Astrophysics Data System (ADS)
Monozon, B. S.; Schmelcher, P.
2017-02-01
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.
Etzold, Fabian; Howard, Ian A; Mauer, Ralf; Meister, Michael; Kim, Tae-Dong; Lee, Kwang-Sup; Baek, Nam Seob; Laquai, Frédéric
2011-06-22
that then contribute to the extracted photocurrent. Despite the high yield of free charges the power conversion efficiency of devices remains moderate at about 3.0%. This is largely a consequence of the low fill factor of devices. We relate the low fill factor to significant energetic disorder present in the pristine polymer and in the polymer:fullerene blends. In the former we observed a significant spectral relaxation of exciton emission (fluorescence) and in the latter of the polaron-induced ground-state bleaching, implying that the density of states (DOS) for both excitons and charge carriers is significantly broadened by energetic disorder in pristine PCDTBT and in its blend with PCBM. This disorder leads to charge trapping in solar cells, which in turn causes higher carrier concentrations and more significant nongeminate recombination. The nongeminate recombination has a significant impact on the IV curves of devices, namely its competition with charge carrier extraction causes a stronger bias dependence of the photocurrent of devices, in turn leading to the poor device fill factor. In addition our results demonstrate the importance of ultrafast free carrier generation and suppression of interfacial CT-state formation and question the applicability of the often used Braun-Onsager model to describe the bias dependence of the photocurrent in polymer:fullerene organic photovoltaic devices.
Taming excitons in II-VI semiconductor nanowires and nanobelts
NASA Astrophysics Data System (ADS)
Xu, Xinlong; Zhang, Qing; Zhang, Jun; Zhou, Yixuan; Xiong, Qihua
2014-10-01
Excitons are one of the most important fundamental quasi-particles, and are involved in a variety of processes forming the basis of a wide range of opto-electronic and photonic devices based on II-VI semiconductor nanowires and nanobelts, such as light-emitting diodes, photovoltaic cells, photodetectors and nanolasers. A clear understanding of their properties and unveiling the potential engineering for excitons is of particular importance for the design and optimization of nanoscale opto-electronic and photonic devices. Herein, we present a comprehensive review on discussing the fundamental behaviours of the excitons in one-dimensional (1D) II-VI semiconductor nanomaterials (nanowires and nanobelts). We will start with a focus on the unique properties (origin, generation, etc) and dynamics of excitons and exciton complexes in the II-VI semiconductor nanowires and nanobelts. Then we move to the recent progress on the excitonic response in 1D nanomaterials and focus on the tailoring and engineering of excitonic properties through rational controlling of the physical parameters and conditions, intrinsically and extrinsically. These include (1) exciton-exciton interaction, which is important for 1D nanomaterial nanolasing; (2) exciton-phonon interaction, which has interesting applications for laser cooling; and (3) exciton-plasmon interaction, which is the cornerstone towards the realization of plasmonic lasers. The potential of electric field, morphology and size control for excitonic properties is also discussed. Unveiling and controlling excitonic properties in II-VI semiconductor nanowires and nanobelts would promote the development of 1D nanoscience and nanotechnology.
Final Report, DOE grant DE-FG02-99ER45780, "Indirect Excitons in Coupled Quantum Wells"
Snoke, david W.
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.
Two-dimensional coherent spectroscopy of excitons, biexcitons, and exciton-polaritons
NASA Astrophysics Data System (ADS)
Bristow, Alan D.
2016-10-01
Semiconductors systems exhibiting excitonic properties are discussed in terms of their coherent response, which is extracted using two-dimensional coherent spectroscopy. This control method allows for separation of quantum pathways that comprise the optical response, such as interactions between excitons, their dephasing rates, the effects of many-body interactions and the role of structure on the microscopic electronic environment. Additional controls, such as polarization can be used to further distinguish biexcitons and suppress many-body interactions. These result are compared and contrasted with those from a semiconductor microcavity where the excitons form polaritonic modes due to normal-mode splitting. Rephrasing spectra map the detuning dependence of the exciton-polariton branches. Increasing the detuning shifts all features to higher energy and the expected anti-crossing is observed. An isolated biexciton is seen only at negative detuning, separated by a binding energy. For positive detuning, the spectral weight of the off-diagonal features swap, as the lower polariton branch and biexciton come into resonance. This indicates that the off-diagonal features are sensitive to the interactions of the exciton-polaritons and other resonances in the system.
Optical properties of MgZnO alloys: Excitons and exciton-phonon complexes
Neumann, M. D.; Cobet, C.; Esser, N.; Laumer, B.; Wassner, T. A.; Eickhoff, M.; Feneberg, M.; Goldhahn, R.
2011-07-01
The characteristics of the excitonic absorption and emission around the fundamental bandgap of wurtzite Mg{sub x}Zn{sub 1-x}O grown on c-plane sapphire substrates by plasma assisted molecular beam epitaxy with Mg contents between x = 0 and x = 0.23 are studied using spectroscopic ellipsometry and photoluminescence (PL) measurements. The ellipsometric data were analyzed using a multilayer model yielding the dielectric function (DF). The imaginary part of the DF for the alloys exhibits a pronounced feature which is attributed to exciton-phonon coupling (EPC) similar to the previously reported results for ZnO. Thus, in order to determine reliable transition energies, the spectral dependence is analyzed by a model which includes free excitonic lines, the exciton continuum, and the enhanced absorption due to EPC. A line shape analysis of the temperature-dependent PL spectra yielded in particular the emission-related free excitonic transition energies, which are compared to the results from the DF line-shape analysis. The PL linewidth is discussed within the framework of an alloy disorder model.
Proposal for dark exciton based chemical sensors
NASA Astrophysics Data System (ADS)
Feierabend, Maja; Berghäuser, Gunnar; Knorr, Andreas; Malic, Ermin
2017-03-01
The rapidly increasing use of sensors throughout different research disciplines and the demand for more efficient devices with less power consumption depends critically on the emergence of new sensor materials and novel sensor concepts. Atomically thin transition metal dichalcogenides have a huge potential for sensor development within a wide range of applications. Their optimal surface-to-volume ratio combined with strong light-matter interaction results in a high sensitivity to changes in their surroundings. Here, we present a highly efficient sensing mechanism to detect molecules based on dark excitons in these materials. We show that the presence of molecules with a dipole moment transforms dark states into bright excitons, resulting in an additional pronounced peak in easy accessible optical spectra. This effect exhibits a huge potential for sensor applications, since it offers an unambiguous optical fingerprint for the detection of molecules--in contrast to common sensing schemes relying on small peak shifts and intensity changes.
Multiple Exciton Generation in Colloidal Nanocrystals
Smith, Charles; Binks, David
2013-01-01
In a conventional solar cell, the energy of an absorbed photon in excess of the band gap is rapidly lost as heat, and this is one of the main reasons that the theoretical efficiency is limited to ~33%. However, an alternative process, multiple exciton generation (MEG), can occur in colloidal quantum dots. Here, some or all of the excess energy is instead used to promote one or more additional electrons to the conduction band, potentially increasing the photocurrent of a solar cell and thereby its output efficiency. This review will describe the development of this field over the decade since the first experimental demonstration of multiple exciton generation, including the controversies over experimental artefacts, comparison with similar effects in bulk materials, and the underlying mechanisms. We will also describe the current state-of-the-art and outline promising directions for further development.
Emission of Tamm plasmon/exciton polaritons
NASA Astrophysics Data System (ADS)
Symonds, C.; Lemaître, A.; Homeyer, E.; Plenet, J. C.; Bellessa, J.
2009-10-01
We report on the observation of the strong coupling regime occurring between a Tamm plasmon (TP) mode and an exciton from inorganic quantum wells (QWs). The sample is formed by a silver thin film deposited onto an AlAs/GaAlAs Bragg reflector containing InGaAs QWs located in the high refractive index layers. Angular resolved reflectometry experiments evidence a clear anticrossing in the dispersion relations, a signature of the strong coupling regime. The Rabi splitting energy is 11.5 meV. The experimental data are in very good agreement with simple transfer matrix calculations. The emission from low and high energy TP/exciton polaritons is also demonstrated.
Polaron pair mediated triplet generation in polymer/fullerene blends
Dimitrov, Stoichko D.; Wheeler, Scot; Niedzialek, Dorota; Schroeder, Bob C.; Utzat, Hendrik; Frost, Jarvist M.; Yao, Jizhong; Gillett, Alexander; Tuladhar, Pabitra S.; McCulloch, Iain; Nelson, Jenny; Durrant, James R.
2015-01-01
Electron spin is a key consideration for the function of organic semiconductors in light-emitting diodes and solar cells, as well as spintronic applications relying on organic magnetoresistance. A mechanism for triplet excited state generation in such systems is by recombination of electron-hole pairs. However, the exact charge recombination mechanism, whether geminate or nongeminate and whether it involves spin-state mixing is not well understood. In this work, the dynamics of free charge separation competing with recombination to polymer triplet states is studied in two closely related polymer-fullerene blends with differing polymer fluorination and photovoltaic performance. Using time-resolved laser spectroscopic techniques and quantum chemical calculations, we show that lower charge separation in the fluorinated system is associated with the formation of bound electron-hole pairs, which undergo spin-state mixing on the nanosecond timescale and subsequent geminate recombination to triplet excitons. We find that these bound electron-hole pairs can be dissociated by electric fields. PMID:25735188
Resonant pairing of excitons in semiconductor heterostructures
NASA Astrophysics Data System (ADS)
Andreev, S. V.
2016-10-01
We suggest indirect excitons in two-dimensional semiconductor heterostructures as a platform for the realization of a bosonic analog of the Bardeen-Cooper-Schrieffer superconductor. The quantum phase transition to a biexcitonic gapped state can be controlled in situ by tuning the electric field applied to the structure in the growth direction. The proposed playground should allow one to go to strongly correlated and high-temperature regimes, unattainable with Feshbach resonant atomic gases.
Excitonic effects in oxyhalide scintillating host compounds
Shwetha, G.; Kanchana, V.; Valsakumar, M. C.
2014-10-07
Ab-initio calculations based on density functional theory have been performed to study the electronic, optical, mechanical, and vibrational properties of scintillator host compounds YOX (X = F, Cl, Br, and I). Semiempirical dispersion correction schemes are used to find the effect of van der Waals forces on these layered compounds and we found this effect to be negligible except for YOBr. Calculations of phonons and elastic constants showed that all the compounds studied here are both dynamically and mechanically stable. YOF and YOI are found to be indirect band gap insulators while YOCl and YOBr are direct band gap insulators. The band gap is found to decrease as we move from fluorine to iodine, while the calculated refractive index shows the opposite trend. As the band gap decreases on going down the periodic table from YOF to YOI, the luminescence increases. The excitonic binding energy calculated, within the effective mass approximation, is found to be more for YOF than the remaining compounds, suggesting that the excitonic effect to be more in YOF than the other compounds. The optical properties are calculated within the Time-Dependent Density Functional Theory (TDDFT) and compared with results obtained within the random phase approximation. The TDDFT calculations, using the newly developed bootstrap exchange-correlation kernel, showed significant excitonic effects in all the compounds studied here.
Valley excitons in two-dimensional semiconductors
Yu, Hongyi; Cui, Xiaodong; Xu, Xiaodong; Yao, Wang
2014-12-30
Monolayer group-VIB transition metal dichalcogenides have recently emerged as a new class of semiconductors in the two-dimensional limit. The attractive properties include: the visible range direct band gap ideal for exploring optoelectronic applications; the intriguing physics associated with spin and valley pseudospin of carriers which implies potentials for novel electronics based on these internal degrees of freedom; the exceptionally strong Coulomb interaction due to the two-dimensional geometry and the large effective masses. The physics of excitons, the bound states of electrons and holes, has been one of the most actively studied topics on these two-dimensional semiconductors, where the excitons exhibit remarkably new features due to the strong Coulomb binding, the valley degeneracy of the band edges, and the valley dependent optical selection rules for interband transitions. Here we give a brief overview of the experimental and theoretical findings on excitons in two-dimensional transition metal dichalcogenides, with focus on the novel properties associated with their valley degrees of freedom.
Valley excitons in two-dimensional semiconductors
Yu, Hongyi; Cui, Xiaodong; Xu, Xiaodong; ...
2014-12-30
Monolayer group-VIB transition metal dichalcogenides have recently emerged as a new class of semiconductors in the two-dimensional limit. The attractive properties include: the visible range direct band gap ideal for exploring optoelectronic applications; the intriguing physics associated with spin and valley pseudospin of carriers which implies potentials for novel electronics based on these internal degrees of freedom; the exceptionally strong Coulomb interaction due to the two-dimensional geometry and the large effective masses. The physics of excitons, the bound states of electrons and holes, has been one of the most actively studied topics on these two-dimensional semiconductors, where the excitons exhibitmore » remarkably new features due to the strong Coulomb binding, the valley degeneracy of the band edges, and the valley dependent optical selection rules for interband transitions. Here we give a brief overview of the experimental and theoretical findings on excitons in two-dimensional transition metal dichalcogenides, with focus on the novel properties associated with their valley degrees of freedom.« less
Microcavity controlled coupling of excitonic qubits.
Albert, F; Sivalertporn, K; Kasprzak, J; Strauß, M; Schneider, C; Höfling, S; Kamp, M; Forchel, A; Reitzenstein, S; Muljarov, E A; Langbein, W
2013-01-01
Controlled non-local energy and coherence transfer enables light harvesting in photosynthesis and non-local logical operations in quantum computing. This process is intuitively pictured by a pair of mechanical oscillators, coupled by a spring, allowing for a reversible exchange of excitation. On a microscopic level, the most relevant mechanism of coherent coupling of distant quantum bits--like trapped ions, superconducting qubits or excitons confined in semiconductor quantum dots--is coupling via the electromagnetic field. Here we demonstrate the controlled coherent coupling of spatially separated quantum dots via the photon mode of a solid state microresonator using the strong exciton-photon coupling regime. This is enabled by two-dimensional spectroscopy of the sample's coherent response, a sensitive probe of the coherent coupling. The results are quantitatively understood in a rigorous description of the cavity-mediated coupling of the quantum dot excitons. This mechanism can be used, for instance in photonic crystal cavity networks, to enable a long-range, non-local coherent coupling.
Singlet exciton fission in nanostructured organic solar cells.
Jadhav, Priya J; Mohanty, Aseema; Sussman, Jason; Lee, Jiye; Baldo, Marc A
2011-04-13
Singlet exciton fission is an efficient multiexciton generation process in organic molecules. But two concerns must be satisfied before it can be exploited in low-cost solution-processed organic solar cells. Fission must be combined with longer wavelength absorption in a structure that can potentially surpass the single junction limit, and its efficiency must be demonstrated in nanoscale domains within blended devices. Here, we report organic solar cells comprised of tetracene, copper phthalocyanine, and the buckyball C(60). Short wavelength light generates singlet excitons in tetracene. These are subsequently split into two triplet excitons and transported through the phthalocyanine. In addition, the phthalocyanine absorbs photons below the singlet exciton energy of tetracene. To test tetracene in nanostructured blends, we fabricate coevaporated bulk heterojunctions and multilayer heterojunctions of tetracene and C(60). We measure a singlet fission efficiency of (71 ± 18)%, demonstrating that exciton fission can efficiently compete with exciton dissociation on the nanoscale.
Bose-Einstein condensation of dipolar excitons in quantum wells
NASA Astrophysics Data System (ADS)
Timofeev, V. B.; Gorbunov, A. V.
2009-02-01
The experiments on Bose-Einstein condensation (BEC) of dipolar (spatially-indirect) excitons in the lateral traps in GaAs/AlGaAs Schottky-diode heterostructures with double and single quantum wells are presented. The condensed part of dipolar excitons under detection in the far zone is placed in k-space in the range which is almost two orders of magnitude less than thermal exciton wave vector. BEC occurs spontaneously in a reservoir of thermalized excitons. Luminescence images of Bose-condensate of dipolar excitons exhibit along perimeter of circular trap axially symmetrical spatial structures of equidistant bright spots which strongly depend on excitation power and temperature. By means of two-beam interference experiments with the use of cw and pulsed photoexcitation it was found that the state of dipolar exciton Bose-condensate is spatially coherent and the whole patterned luminescence configuration in real space is described by a common wave function.
Excitonic Stark effect in MoS2 monolayers
NASA Astrophysics Data System (ADS)
Scharf, Benedikt; Frank, Tobias; Gmitra, Martin; Fabian, Jaroslav; Žutić, Igor; Perebeinos, Vasili
2016-12-01
We theoretically investigate excitons in MoS2 monolayers in an applied in-plane electric field. Tight-binding and Bethe-Salpeter equation calculations predict a quadratic Stark shift, of the order of a few meV for fields of 10 V/μ m , in the linear absorption spectra. The spectral weight of the main exciton peaks decreases by a few percent with an increasing electric field due to the exciton field ionization into free carriers as reflected in the exciton wave functions. Subpicosecond exciton decay lifetimes at fields of a few tens of V/μ m could be utilized in solar energy harvesting and photodetection. We find simple scaling relations of the exciton binding, radius, and oscillator strength with the dielectric environment and an electric field, which provides a path to engineering the MoS2 electro-optical response.
Hybrid states of Tamm plasmons and exciton-polaritons
NASA Astrophysics Data System (ADS)
Kaliteevski, M.; Brand, S.; Abram, R. A.; Iorsh, I.; Kavokin, A. V.; Liew, T. C. H.; Shelykh, I. A.
2011-03-01
We have demonstrated theoretically that it is possible to use the resonant coupling of exciton-polaritons in a planar microcavity and Tamm plasmons at a metal film on the surface of the structure to provide lateral spatial control of the exciton-polaritons within the cavity. The resonant coupling of the Tamm plasmons to cavity exciton-polaritons results in a triplet of hybrid plasmon-exciton-polariton modes with the lowest at a significantly lower energy than that of the unperturbed exciton-polaritons. Further, a patterned metal film on the structure surface can provide a sufficiently large lateral modulation of the excitation energy that localization of the exciton-polaritons within chosen regions of the cavity is possible. We show how the approach opens the way to a practical demonstration of polariton channels, traps, and devices, including logic gates.
Excitonic gap formation and condensation in the bilayer graphene structure
NASA Astrophysics Data System (ADS)
Apinyan, V.; Kopeć, T. K.
2016-09-01
We have studied the excitonic gap formation in the Bernal Stacked, bilayer graphene (BLG) structures at half-filling. Considering the local Coulomb interaction between the layers, we calculate the excitonic gap parameter and we discuss the role of the interlayer and intralayer Coulomb interactions and the interlayer hopping on the excitonic pair formation in the BLG. Particularly, we predict the origin of excitonic gap formation and condensation, in relation to the furthermost interband optical transition spectrum. The general diagram of excitonic phase transition is given, explaining different interlayer correlation regimes. The temperature dependence of the excitonic gap parameter is shown and the role of the chemical potential, in the BLG, is discussed in details.
Spin-charge order and excitonic effects in sawtooth-like graphene nanoribbons
NASA Astrophysics Data System (ADS)
Wu, Sha; Lu, Wengang; Qi, Jingshan
2016-09-01
In this paper we systematically study electronic structures and excitonic effects in one type of the sawtooth-like graphene nanoribbons. A main feature is that the local magnetism is developed for the certain width and changes with the increase of width. A variety of magnetic orders root in the competition of the short range interaction between the same spin-electrons and long range exchange interaction between opposite spin-electrons. For excitonic effects, the binding energy of degenerate spin-triplets T1 and T-1 is higher than that of T0 for all studied nanoribbons and is size dependent. We reveal the underlying physical mechanism from the charge distributions of excitons and its correlation with the spin-resolved charge density distributions in the ground state. We find that the electrons and holes in degenerate spin-triplets T1 and T-1 are closer together and thus the interaction between them is more strong, while the distribution of electrons and holes is relatively more disperse for T0, indicating the weaker interaction. We hope that these interesting results are able to be detected in the experiment and these multi-performance samples are better utilized in future device applications.
Excitonic Aharonov-Bohm effect in a two-dimensional quantum ring
Gonzalez-Santander, C.; Dominguez-Adame, F.; Roemer, R. A.
2011-12-15
We study theoretically the optical properties of an exciton in a two-dimensional ring threaded by a magnetic flux. We model the quantum ring by a confining potential that can be continuously tuned from strictly one-dimensional to truly two-dimensional with finite radius-to-width ratio. We present an analytic solution of the problem when the electron-hole interaction is short ranged. The oscillatory dependence of the oscillator strength as a function of the magnetic flux is attributed to the Aharonov-Bohm effect. The amplitude of the oscillations changes upon increasing the width of the quantum ring. We find that the Aharonov-Bohm oscillations of the ground state of the exciton decrease with increasing the width, but, remarkably, the amplitude remains finite down to radius-to-width ratios less than unity. We attribute this resilience of the excitonic oscillations to the nonsimple connectedness of our chosen confinement potential with its centrifugal core at the origin.
Cobet, Christoph; Gasiorowski, Jacek; Menon, Reghu; Hingerl, Kurt; Schlager, Stefanie; White, Matthew S.; Neugebauer, Helmut; Sariciftci, N. Serdar; Stadler, Philipp
2016-01-01
Electron-phonon interactions of free charge-carriers in doped pi-conjugated polymers are conceptually described by 1-dimensional (1D) delocalization. Thereby, polaronic transitions fit the 1D-Froehlich model in quasi-confined chains. However, recent developments in conjugated polymers have diversified the backbones to become elaborate heterocylcic macromolecules. Their complexity makes it difficult to investigate the electron-phonon coupling. In this work we resolve the electron-phonon interactions in the ground and doped state in a complex push-pull polymer. We focus on the polaronic transitions using in-situ spectroscopy to work out the differences between single-unit and push-pull systems to obtain the desired structural- electronic correlations in the doped state. We apply the classic 1D-Froehlich model to generate optical model fits. Interestingly, we find the 1D-approach in push-pull polarons in agreement to the model, pointing at the strong 1D-character and plain electronic structure of the push-pull structure. In contrast, polarons in the single-unit polymer emerge to a multi- dimensional problem difficult to resolve due to their anisotropy. Thus, we report an enhancement of the 1D-character by the push-pull concept in the doped state - an important view in light of the main purpose of push-pull polymers for photovoltaic devices. PMID:27731421
Polaron effect on the optical rectification in spherical quantum dots with electric field
NASA Astrophysics Data System (ADS)
Feng, Zhen-Yu; Yan, Zu-Wei
2016-10-01
The polaron effect on the optical rectification in spherical quantum dots with a shallow hydrogenic impurity in the presence of electric field is theoretically investigated by taking into account the interactions of the electrons with both confined and surface optical phonons. Besides, the interaction between impurity and phonons is also considered. Numerical calculations are presented for typical Zn1-x Cd x Se/ZnSe material. It is found that the polaronic effect or electric field leads to the redshifted resonant peaks of the optical rectification coefficients. It is also found that the peak values of the optical rectification coefficients with the polaronic effect are larger than without the polaronic effect, especially for smaller Cd concentrations or stronger electric field. Project supported by the National Natural Science Foundation of China (Grant No. 11364028), the Major Projects of the Natural Science Foundation of Inner Mongolia Autonomous Region, China (Grant No. 2013ZD02), and the Project of “Prairie Excellent” Engineering in Inner Mongolia Autonomous Region, China.
Optical polaron effect on the electronic states of a heterojunction potential
NASA Astrophysics Data System (ADS)
Ban, S. L.; Hasbun, J. E.
1997-11-01
The polaron effect contribution to the electronic ground state in a heterojunction potential is investigated by considering the bulk and the interface phonons influence. A self-consistent heterojunction potential is used and an LLP-like method is used to obtain the polaron effect. The GaAs/Al_xGa_1-xAs (0.3
NASA Astrophysics Data System (ADS)
Cobet, Christoph; Gasiorowski, Jacek; Menon, Reghu; Hingerl, Kurt; Schlager, Stefanie; White, Matthew S.; Neugebauer, Helmut; Sariciftci, N. Serdar; Stadler, Philipp
2016-10-01
Electron-phonon interactions of free charge-carriers in doped pi-conjugated polymers are conceptually described by 1-dimensional (1D) delocalization. Thereby, polaronic transitions fit the 1D-Froehlich model in quasi-confined chains. However, recent developments in conjugated polymers have diversified the backbones to become elaborate heterocylcic macromolecules. Their complexity makes it difficult to investigate the electron-phonon coupling. In this work we resolve the electron-phonon interactions in the ground and doped state in a complex push-pull polymer. We focus on the polaronic transitions using in-situ spectroscopy to work out the differences between single-unit and push-pull systems to obtain the desired structural- electronic correlations in the doped state. We apply the classic 1D-Froehlich model to generate optical model fits. Interestingly, we find the 1D-approach in push-pull polarons in agreement to the model, pointing at the strong 1D-character and plain electronic structure of the push-pull structure. In contrast, polarons in the single-unit polymer emerge to a multi- dimensional problem difficult to resolve due to their anisotropy. Thus, we report an enhancement of the 1D-character by the push-pull concept in the doped state - an important view in light of the main purpose of push-pull polymers for photovoltaic devices.
Generalized Hartree-Fock-Bogoliubov description of the Fröhlich polaron
NASA Astrophysics Data System (ADS)
Kain, Ben; Ling, Hong Y.
2016-07-01
We adapt the generalized Hartree-Fock-Bogoliubov (HFB) method to an interacting many-phonon system free of impurities. The many-phonon system is obtained from applying the Lee-Low-Pine (LLP) transformation to the Fröhlich model which describes a mobile impurity coupled to noninteracting phonons. We specialize our general HFB description of the Fröhlich polaron to Bose polarons in quasi-one-dimensional cold-atom mixtures. The LLP-transformed many-phonon system distinguishes itself with an artificial phonon-phonon interaction which is very different from the usual two-body interaction. We use the quasi-one-dimensional model, which is free of an ultraviolet divergence that exists in higher dimensions, to better understand how this unique interaction affects polaron states and how the density and pair correlations inherent to the HFB method conspire to create a polaron ground state with an energy in good agreement with and far closer to the prediction from Feynman's variational path integral approach than mean-field theory where HFB correlations are absent.
Emin, David
2016-01-28
Charge carriers that execute multi-phonon hopping generally interact strongly enough with phonons to form polarons. A polaron's sluggish motion is linked to slowly shifting atomic displacements that severely reduce the intrinsic width of its transport band. Here a means to estimate hopping polarons' bandwidths from Seebeck-coefficient measurements is described. The magnitudes of semiconductors' Seebeck coefficients are usually quite large (>k/|q| = 86 μV/K) near room temperature. However, in accord with the third law of thermodynamics, Seebeck coefficients must vanish at absolute zero. Here, the transition of the Seebeck coefficient of hopping polarons to its low-temperature regime is investigated. The temperature and sharpness of this transition depend on the concentration of carriers and on the width of their transport band. This feature provides a means of estimating the width of a polaron's transport band. Since the intrinsic broadening of polaron bands is very small, less than the characteristic phonon energy, the net widths of polaron transport bands in disordered semiconductors approach the energetic disorder experienced by their hopping carriers, their disorder energy.
NASA Astrophysics Data System (ADS)
Madrid, Angeline; Kim, Hyeon-Deuk; Habenicht, Bradley; Prezhdo, Oleg
2010-03-01
Phonon-induced dephasing processes that govern optical line widths, multiple exciton (ME) generation (MEG), and ME fission (MEF) in semiconductor quantum dots (QDs) are investigated by ab initio molecular dynamics simulation. Using Si QDs as an example, we propose that MEF occurs by phonon-induced dephasing and, for the first time, estimate its time scale to be 100 fs. In contrast, luminescence and MEG dephasing times are all sub-10 fs. Generally, dephasing is faster for higher-energy and higher-order excitons and increased temperatures. MEF is slow because it is facilitated only by low-frequency acoustic modes. Luminescence and MEG couple to both acoustic and optical modes of the QD, as well as ligand vibrations. The detailed atomistic simulation of the dephasing processes advances understanding of exciton dynamics in QDs and other nanoscale materials.
Plasmon-Frenkel-exciton in a clustered solid
NASA Astrophysics Data System (ADS)
Rotkin, Slava V.; Suris, Robert A.
1998-08-01
The standard theory of the Frenkel exciton (a small radius exciton) is applied to a fullerene 2D solid. It is the dipole collective electron excitation of a single cluster which forms the delocalized plasmon-Frenkel-exciton (PFE) in a crystal. The PFE retarded interaction is taken into account. We present transverse PFE-polariton dispersion curves along with the Coulomb problem solution for longitudinal excitation in the 2D plane.
Spatially indirect exciton condensate phases in double bilayer graphene
NASA Astrophysics Data System (ADS)
Su, Jung-Jung; MacDonald, Allan H.
2017-01-01
We present a theory of spatially indirect exciton condensate states in systems composed of a pair of electrically isolated Bernal graphene bilayers. The ground-state phase diagram in a two-dimensional displacement-field/inter-bilayer-bias space includes layer-polarized semiconductors, spin-density-wave states, exciton condensates, and states with mixed excitonic and spin order. We find that two different condensate states, distinguished by a chirality index, are stable under different electrical control conditions.
Photogenerated exciton dissociation in highly coupled lead salt nanocrystal assemblies.
Choi, Joshua J; Luria, Justin; Hyun, Byung-Ryool; Bartnik, Adam C; Sun, Liangfeng; Lim, Yee-Fun; Marohn, John A; Wise, Frank W; Hanrath, Tobias
2010-05-12
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.
Field-induced exciton condensation in LaCoO3
Sotnikov, A.; Kuneš, J.
2016-01-01
Motivated by recent observation of magnetic field induced transition in LaCoO3 we study the effect of external field in systems close to instabilities towards spin-state ordering and exciton condensation. We show that, while in both cases the transition can be induced by an external field, temperature dependencies of the critical field have opposite slopes. Based on this result we argue that the experimental observations select the exciton condensation scenario. We show that such condensation is possible due to high mobility of the intermediate spin excitations. The estimated width of the corresponding dispersion is large enough to overrule the order of atomic multiplets and to make the intermediate spin excitation propagating with a specific wave vector the lowest excitation of the system. PMID:27461512
Phase diagram for the trapping kinetics of partially coherent excitons
NASA Astrophysics Data System (ADS)
Pearlstein, Robert M.
1998-06-01
The kinetics of exciton trapping within molecular assemblies similar to those of recently reported structural models of photosynthetic light-harvesting antennas have been described theoretically for any degree of exciton coherence. It is shown here that in the space of two of the kinetic parameters - the local exciton scattering rate constant and the nearest-neighbor separation distance of the exciton-generating transition dipoles - the trapping kinetics segregate into coherent and incoherent phases delineated by universal curves. Consequences of these findings are discussed, particularly as they may apply to purple photosynthetic bacteria.
Surface photovoltage in exciton absorption range in CdS
NASA Technical Reports Server (NTRS)
Morawski, A.; Banisch, R.; Lagowski, J.
1977-01-01
The high resolution, intrinsic spectra of surface photovoltage are reported for semiconducting n-type CdS single crystals. At reduced temperatures (120-160 K) the spectra exhibit three sharp maxima due to A, B and C free exciton transitions. Energy positions of these lines and valence band parameters (spin-orbit and crystal field splittings) estimated from surface photovoltage are in good agreement with values obtained by other methods. The excitonic transitions are very sensitive to surface treatment, i.e. polishing, etching, background illumination and surface doping. The mechanism of direct interaction of free excitons with surface states is proposed to explain exciton lines in surface photovoltage.
Exciton management in organic photovoltaic multidonor energy cascades.
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.
Simulations of singlet exciton diffusion in organic semiconductors: a review
Bjorgaard, Josiah A.; Kose, Muhammet Erkan
2014-12-22
Our review describes the various aspects of simulation strategies for exciton diffusion in condensed phase thin films of organic semiconductors. Several methods for calculating energy transfer rate constants are discussed along with procedures for how to account for energetic disorder. Exciton diffusion can be modelled by using kinetic Monte-Carlo methods or master equations. Recent literature on simulation efforts for estimating exciton diffusion lengths of various conjugated polymers and small molecules are introduced. Moreover, these studies are discussed in the context of the effects of morphology on exciton diffusion and the necessity of accurate treatment of disorder for comparison of simulation results with those of experiment.
Multiple exciton generation and recombination in carbon nanotubes and nanocrystals.
Kanemitsu, Yoshihiko
2013-06-18
Semiconducting nanomaterials such as single-walled carbon nanotubes (SWCNTs) and nanocrystals (NCs) exhibit unique size-dependent quantum properties. They have therefore attracted considerable attention from the viewpoints of fundamental physics and functional device applications. SWCNTs and NCs also provide an excellent new stage for experimental studies of many-body effects of electrons and excitons on optical processes in nanomaterials. In this Account, we discuss multiple exciton generation and recombination in SWCNTs and NCs for next-generation photovoltaics. Strongly correlated ensembles of conduction-band electrons and valence-band holes in semiconductors are complex quantum systems that exhibit unique optical phenomena. In bulk crystals, the carrier recombination dynamics can be described by a simple model, which includes the nonradiative single-carrier trapping rate, the radiative two-carrier recombination rate, and the nonradiative three-carrier Auger recombination rate. The nonradiative Auger recombination rate determines the carrier recombination dynamics at high carrier density and depends on the spatial localization of carriers in two-dimensional quantum wells. The Auger recombination and multiple exciton generation rates can be advantageously manipulated by nanomaterials with designated energy structures. In addition, SWCNTs and NCs show quantized recombination dynamics of multiple excitons and carriers. In one-dimensional SWCNTs, excitons have large binding energies and are very stable at room temperature. The extremely rapid Auger recombination between excitons determines the photoluminescence (PL) intensity, the PL linewidth, and the PL lifetime. SWCNTs can undergo multiple exciton generation, while strong exciton-exciton interactions and complicated exciton structures affect the quantized Auger rate and the multiple exciton generation efficiency. Interestingly, in zero-dimensional NC quantum dots, quantized Auger recombination causes unique
Excitons and multi-excitons in single CdTe quantum dots probed by near-field spectroscopy
NASA Astrophysics Data System (ADS)
Brun, M.; Huant, S.; Woehl, J. C.; Motte, J.-F.; Marsal, L.; Mariette, H.
2002-03-01
A near-field optical spectroscopy study of a single CdTe/ZnTe quantum dot at low temperatures is presented. While the photoluminescence spectrum at low excitation power reveals only one single sharp peak due to the radiative recombination of excitons (X) in the single dot, several additional sharp peaks appear with increasing excitation density. The dominant features are ascribed to exciton complexes and charged exciton complexes such as negatively charged excitons (X -), neutral (2X and 3X) and negative (2X - and 3X -) biexcitons and triexcitons. Exciton charging arises due to efficient hole trapping by residual acceptors in the barrier material. This partly inhibits the formation of biexcitons and triexcitons. A spectral feature appearing close to the X - peak is tentatively assigned to X 2- negative excitons. This feature is found to shift to the red with increasing power: two possible explanations for this unexpected behaviour are proposed.
Polaron dynamics in two types of long oligothiophenes revealed by Q - and X -band ESR measurements
NASA Astrophysics Data System (ADS)
Kanemoto, Katsuichi; Furukawa, Ko; Negishi, Nobukazu; Aso, Yoshio; Otsubo, Tetsuo
2007-10-01
The polaron dynamics has been investigated through the X - and Q -band ESR measurements for two types of iodine-doped long oligothiophenes, the 20-mer with octyl substituents (o-20T) and the 16-mer with hexyl substituents (h-16T) . o-20T , used as a model compound of conjugated polymers with crystalline grains, gives anisotropic ESR spectra attributed to g anisotropy at low temperatures. The anisotropic spectra are found to be brought by polarons moving within the crystalline grains consisting of parallel chains. The anisotropy is shown to decrease with increasing temperature. This provides definite evidence that the polarons transfer among some grains by the assist of temperature. In contrast, h-16T , used as a model of the polymers with amorphous morphology, gives almost isotropic ESR spectra even in the Q -band measurement. This feature of h-16T is explained to be caused by a rapid interchain transfer of polarons. Spectral simulations performed for obtained spectra reveal that the ESR linewidth in the Q -band measurement is larger than that in the X band for both oligothiophenes. The difference of the linewidth is analyzed by a simplified motional narrowing model in order to draw the information of polaron dynamics. Analyses for o-20T show that the intergrain motion almost follows the variable range hopping model. The interchain motion in h-16T is found to have a much weaker temperature dependence than the intergrain motion in o-20T . This result suggests that the interchain dynamics of h-16T revealed by the ESR technique includes a variety of processes of motion.
Miyamoto, Satoru; Ishikawa, Toyofumi; Eto, Mikio; Itoh, Kohei M.; Moutanabbir, Oussama; Haller, Eugene E.; Sawano, Kentarou; Shiraki, Yasuhiro
2010-08-15
We report on a magnetophotoluminescence study of isotopically pure {sup 70}Ge/Si self-assembled type-II quantum dots. Oscillatory behaviors attributed to the Aharonov-Bohm effect are simultaneously observed for the emission energy and intensity of excitons subject to an increasing magnetic field. When the magnetic flux penetrates through the ringlike trajectory of an electron moving around each quantum dot, the ground state of an exciton experiences a change in its angular momentum. Our results provide the experimental evidence for the phase coherence of localized electron wave functions in group-IV Ge/Si self-assembled quantum structures.
Polaronic Transport in Phosphate Glasses Containing Transition Metal Ions
NASA Astrophysics Data System (ADS)
Henderson, Mark
The goal of this dissertation is to characterize the basic transport properties of phosphate glasses containing various amounts of TIs and to identify and explain any electronic phase transitions which may occur. The P2 O5-V2O5-WO3 (PVW) glass system will be analyzed to find the effect of TI concentration on conduction. In addition, the effect of the relative concentrations of network forming ions (SiO2 and P2O5) on transport will be studied in the P2O5-SiO2-Fe2O 3 (PSF) system. Also presented is a numerical study on a tight-binding model adapted for the purposes of modelling Gaussian traps, mimicking TI's, which are arranged in an extended network. The results of this project will contribute to the development of fundamental theories on the electronic transport in glasses containing mixtures of transition oxides as well as those containing multiple network formers without discernible phase separation. The present study on the PVW follows up on previous investigation into the effect on mixed transition ions in oxide glasses. Past research has focused on glasses containing transition metal ions from the 3d row. The inclusion of tungsten, a 5d transition metal, adds a layer of complexity through the mismatch of the energies of the orbitals contributing to localized states. The data have indicated that a transition reminiscent of a metal-insulator transition (MIT) occurs in this system as the concentration of tungsten increases. As opposed to some other MIT-like transitions found in phosphate glass systems, there seems to be no polaron to bipolaron conversion. Instead, the individual localization parameter for tungsten noticeably decreases dramatically at the transition point as well as the adiabaticity. Another distinctive feature of this project is the study of the PSF system, which contains two true network formers, phosphorous pentoxide (P2O 5) and silicon dioxide (SiO2). It is not usually possible to do a reliable investigation of the conduction properties of
Fu, Ming; Tamarat, Philippe; Huang, He; Even, Jacky; Rogach, Andrey L; Lounis, Brahim
2017-02-27
Revealing the crystal structure of lead halide perovskite nanocrystals is essential for the optimization of stability of these emerging materials in applications such as solar cells, photodetectors and light emitting devices. We use magneto-photoluminescence spectroscopy of individual perovskite CsPbBr3 nanocrystals as a unique tool to determine their crystal structure, which imprints distinct signatures in the excitonic sublevels of charge complexes at low temperatures. At zero magnetic field, the identification of two classes of photoluminescence spectra, displaying either two or three sublevels in their exciton fine structure, shows evidence for the existence of two crystalline structures, namely tetragonal D4h and orthorhombic D2h phases. Magnetic field shifts, splitting and coupling of the sublevels provide a determination of the diamagnetic coefficient and valuable information on the exciton g-factor and its anisotropic character. Moreover, this spectroscopic study reveals the optical properties of charged excitons and allows the extraction of the electron and hole g-factors for perovskite systems.
NASA Astrophysics Data System (ADS)
Elgawadi, Amal; Gainer, Gordon; Krasinski, Jerzy
2013-08-01
The crystal orientation dependence of GaN excitons was investigated via the photoluminescence (PL) technique. The PL emissions at a temperature of 10 K were obtained from two experimental configurations where the emission K vector (the propagation vector) was either parallel (K ∥ c) or perpendicular (K ∥ c) to the crystal c-axis. Longitudinal, transverse and donor-bound excitons were observed in the two configurations. However, the longitudinal excitons converged onto the transverse free exciton Γ5 in the K⊥c emission. This behavior was discussed in terms of electron screening due to the scattering of electrons moving perpendicular to charged dislocation lines. Additionally, the thermal activation energy of the longitudinal excitons was calculated from the temperature dependent PL measurements collected from the K ∥ c emission, and was found to be 5 to 6 times as high as the binding energy of the free excitons. This high energy was interpreted tentatively in view of the creation of polaritons in strong exciton-photon coupling regimes. These findings present fundamental concepts for applications such as vertical cavity surface-emitting lasers (VCSELs) and polariton lasers.
NASA Astrophysics Data System (ADS)
Schröter, M.; Ivanov, S. D.; Schulze, J.; Polyutov, S. P.; Yan, Y.; Pullerits, T.; Kühn, O.
2015-03-01
The influence of exciton-vibrational coupling on the optical and transport properties of molecular aggregates is an old problem that gained renewed interest in recent years. On the experimental side, various nonlinear spectroscopic techniques gave insight into the dynamics of systems as complex as photosynthetic antennae. Striking evidence was gathered that in these protein-pigment complexes quantum coherence is operative even at room temperature conditions. Investigations were triggered to understand the role of vibrational degrees of freedom, beyond that of a heat bath characterized by thermal fluctuations. This development was paralleled by theory, where efficient methods emerged, which could provide the proper frame to perform non-Markovian and non-perturbative simulations of exciton-vibrational dynamics and spectroscopy. This review summarizes the state of affairs of the theory of exciton-vibrational interaction in molecular aggregates and photosynthetic antenna complexes. The focus is put on the discussion of basic effects of exciton-vibrational interaction from the stationary and dynamics points of view. Here, the molecular dimer plays a prominent role as it permits a systematic investigation of absorption and emission spectra by numerical diagonalization of the exciton-vibrational Hamiltonian in a truncated Hilbert space. An extension to larger aggregates, having many coupled nuclear degrees of freedom, becomes possible with the Multi-Layer Multi-Configuration Time-Dependent Hartree (ML-MCTDH) method for wave packet propagation. In fact it will be shown that this method allows one to approach the limit of almost continuous spectral densities, which is usually the realm of density matrix theory. Real system-bath situations are introduced for two models, which differ in the way strongly coupled nuclear coordinates are treated, as a part of the relevant system or the bath. A rather detailed exposition of the Hierarchy Equations Of Motion (HEOM) method will be
Property comparison of polarons in zinc-blende and wurtzite GaN/AlN quantum wells
NASA Astrophysics Data System (ADS)
Jun, Zhu; Shiliang, Ban; Sihua, Ha
2011-11-01
The properties of polarons in zinc-blende and wurtzite GaN/AlN quantum wells with Fröhlich interaction Hamiltonians are compared in detail. The energy shifts of polarons at ground state due to the interface (IF), confined (CO) and half-space phonon modes are calculated by a finite-difference computation combined with a modified LLP variational method. It is found that the two Fröhlich interaction Hamiltonians are consistent with each other when the anisotropic effect from the z-direction and the x-y plane is neglected. The influence of the anisotropy on the polaron energy shifts due to the IF phonon modes for a smaller well width or due to the CO phonon modes for a moderate well width is obvious. In addition, the built-in electric field has a remarkable effect on the polaron energy shifts contributed by the various phonon modes.
NASA Astrophysics Data System (ADS)
Tiotsop, M.; Fotue, A. J.; Fautso, G. K.; Kenfack, C. S.; Fotsin, H. B.; Fai, L. C.
2017-03-01
Using Pekar variational method, Eigen energies of the ground and first excited states of the polaron in triangular bound and Coulomb potential quantum dot are derived in view of investigating the density of probability, the decoherence time and the Shannon entropy. Numerical analysis show that the decoherence time is decreasing function of polaron radius and the strength of the Coulombic impurity and the increase function of dispersion coefficient. These results suggest that the decrease of polaron radius and Coulombic impurity lead to the increase of coherence time. Also the entropy shows the oscillatory periodic evolution as function of the time due to the triangular form of the confinement. It's also seen that entropy is periodic for the lower value of Coulomb impurity parameter and for the higher value of the polaronic radius.
NASA Technical Reports Server (NTRS)
Yeh, N. C.; Vasquez, R. P.; Wei, J. Y. T.; Fu, C. C.; Beach, G.; Huynh, J.; Samoilov, A. V.; Boris, A. V.; Kovaleva, N. N.; Bazhenov, A. V.
1997-01-01
The relevance of lattice distortion, polaron conduction, and double-exchange interaction to the occurrence of colossal magnetoresistance (SMR) is investigated by comparing the physical properties of magnetoresistive manganites and cobaltites.
Excitons and Optical Properties of {alpha} -Quartz
Chang, Eric K.; Rohlfing, Michael; Louie, Steven G. [Department of Physics, University of California at Berkeley, Berkeley, California 94720
2000-09-18
We present an ab initio study of the optical properties of {alpha} -quartz. The absorption spectrum is calculated by solving the Bethe-Salpeter equation for the interacting electron-hole system and found to be in excellent agreement with the measured spectrum up to 10 eV above the absorption threshold. We find that excitonic effects are crucial in understanding the sharp features in the absorption spectrum in this energy range. They are also crucial in the ab initio computation of the static dielectric constant, significantly enhancing its value. (c) 2000 The American Physical Society.
Dynamical excitonic effects in metals and semiconductors.
Marini, Andrea; Del Sole, Rodolfo
2003-10-24
The dynamics of an electron-hole pair induced by the time-dependent screened Coulomb interaction is discussed. In contrast to the case where the static electron-hole interaction is considered we demonstrate the occurrence of important dynamical excitonic effects in the solution of the Bethe-Salpeter equation. This is illustrated in the calculated absorption spectra of noble metals (copper and silver) and silicon. Dynamical corrections strongly affect the spectra, partially canceling dynamical self-energy effects and leading to good agreement with experiment.
Electro-optical properties of Rydberg excitons
NASA Astrophysics Data System (ADS)
Zielińska-Raczyńska, Sylwia; Ziemkiewicz, David; Czajkowski, Gerard
2016-07-01
We show how to compute the electro-optical functions (absorption, reflection, and transmission) when Rydberg exciton-polaritons appear, including the effect of the coherence between the electron-hole pair and the electromagnetic field. With the use of the real density matrix approach, numerical calculations applied for the Cu2O crystal are performed. We also examine in detail and explain the dependence of the resonance displacement on the state number and applied electric field strength. We report a fairly good agreement with recently published experimental data.
Excitonic luminescence upconversion in a two-dimensional semiconductor
Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; ...
2015-12-21
Photon upconversion is an elementary light-matter interaction process in which an absorbed photon is re-emitted at higher frequency after extracting energy from the medium. Furthermore, this phenomenon lies at the heart of optical refrigeration in solids(1), where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities(2) or exciton-phonon coupling(3). We demonstrate a luminescence upconversion process from a negatively charged exciton to a neutral exciton resonance in monolayer WSe2, producing spontaneous anti-Stokes emission with an energy gain of 30 meV. Polarization-resolved measurements find this process to be valley selective, unique to monolayer semiconductors(4). Since the charged exciton binding energy(5) closelymore » matches the 31 meV A(1)' optical phonon(6-9), we ascribe the spontaneous excitonic anti-Stokes to doubly resonant Raman scattering, where the incident and outgoing photons are in resonance with the charged and neutral excitons, respectively. Additionally, we resolve a charged exciton doublet with a 7 meV splitting, probably induced by exchange interactions, and show that anti-Stokes scattering is efficient only when exciting the doublet peak resonant with the phonon, further confirming the excitonic doubly resonant picture.« less
Excitonic luminescence upconversion in a two-dimensional semiconductor
Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; Yan, Jiaqiang; Mandrus, David G.; Taniguchi, Takashi; Watanabe, Kenji; Dery, Hanan; Yao, Wang; Xu, Xiaodong
2015-12-21
Photon upconversion is an elementary light-matter interaction process in which an absorbed photon is re-emitted at higher frequency after extracting energy from the medium. Furthermore, this phenomenon lies at the heart of optical refrigeration in solids(1), where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities(2) or exciton-phonon coupling(3). We demonstrate a luminescence upconversion process from a negatively charged exciton to a neutral exciton resonance in monolayer WSe2, producing spontaneous anti-Stokes emission with an energy gain of 30 meV. Polarization-resolved measurements find this process to be valley selective, unique to monolayer semiconductors(4). Since the charged exciton binding energy(5) closely matches the 31 meV A(1)' optical phonon(6-9), we ascribe the spontaneous excitonic anti-Stokes to doubly resonant Raman scattering, where the incident and outgoing photons are in resonance with the charged and neutral excitons, respectively. Additionally, we resolve a charged exciton doublet with a 7 meV splitting, probably induced by exchange interactions, and show that anti-Stokes scattering is efficient only when exciting the doublet peak resonant with the phonon, further confirming the excitonic doubly resonant picture.
NASA Astrophysics Data System (ADS)
Dimakogianni, M.; Simserides, C.; Triberis, G. P.
2013-07-01
We introduce a theoretical model to scrutinize the conductivity of small polarons in 1D disordered systems, focusing on two crucial - as will be demonstrated - factors: the density of states and the spatial extent of the electronic wave function. The investigation is performed for any temperature up to 300 K and under electric field of arbitrary strength up to the polaron dissociation limit. To accomplish this task, we combine analytical work with numerical calculations.
How to Draw Energy Level Diagrams in Excitonic Solar Cells.
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.
High-Absorption-Efficiency Superlattice Solar Cells by Excitons
NASA Astrophysics Data System (ADS)
Nishinaga, Jiro; Kawaharazuka, Atsushi; Onomitsu, Koji; Horikoshi, Yoshiji
2013-11-01
The effect of excitonic absorption on solar cell efficiency has been investigated using solar cells with AlGaAs/GaAs superlattice structures. Numerical calculations reveal that excitonic absorption considerably enhances the overall absorption of bulk GaAs. Excitonic absorption shows strong and sharp peaks at the absorption edge and in the energy region above the band gap. Absorption enhancement is also achieved in the AlGaAs/GaAs superlattice. The measured quantum efficiency spectra of the superlattice solar cells are quite similar to the calculated absorption spectra considering the excitonic effect. The superlattice solar cells are confirmed to have high absorption coefficient compared with the GaAs and AlGaAs bulk solar cells. These results suggest that the enhanced absorption by excitons can increase the quantum efficiency of solar cells. This effect is more prominent for the solar cells with small absorption layer thicknesses.
Exciton band structure in two-dimensional materials
NASA Astrophysics Data System (ADS)
Cudazzo, Pier Luigi; Sponza, Lorenzo; Giorgetti, Christine; Reining, Lucia; Sottile, Francesco; Gatti, Matteo
In low-dimensional materials the screening of the Coulomb interaction is strongly reduced. As a consequence, the binding energy of both Wannier and Frenkel excitons in the optical spectra is large and comparable in size. Therefore, contrarily to bulk materials, it cannot serve as a criterion to distinguish different kinds of excitons. Here we demonstrate that the exciton band structure, which can be accessed experimentally, instead provides a powerful way to identify the exciton character. By comparing the ab initio solution of the many-body Bethe-Salpeter equation for graphane and single-layer hexagonal BN, we draw a general picture of the exciton dispersion in two-dimensional materials, highlighting the different role played by the exchange electron-hole interaction and by the hopping terms related to the electronic band structure.
Radiative properties of multicarrier bound excitons in GaAs
NASA Astrophysics Data System (ADS)
Karin, Todd; Barbour, Russell J.; Santori, Charles; Yamamoto, Yoshihisa; Hirayama, Yoshiro; Fu, Kai-Mei C.
2015-04-01
Excitons in semiconductors can have multiple lifetimes due to spin-dependent oscillator strengths and interference between different recombination pathways. In addition, strain and symmetry effects can further modify lifetimes via the removal of degeneracies. We present a convenient formalism for predicting the optical properties of k =0 excitons with an arbitrary number of charge carriers in different symmetry environments. Using this formalism, we predict three distinct lifetimes for the neutral acceptor bound exciton in GaAs, and confirm this prediction through polarization dependent and time-resolved photoluminescence experiments. We find the acceptor bound-exciton lifetimes to be To×(1 ,3 ,3/4 ) , where To=(0.61 ±0.12 ) ns . Furthermore, we provide an estimate of the intralevel and interlevel exciton spin-relaxation rates.
Excitons in conjugated polymers: wavefunctions, symmetries, and quantum numbers.
Barford, William; Paiboonvorachat, Nattapong
2008-10-28
We introduce a mapping from configuration interaction singles wavefunctions, expressed as linear combinations of particle-hole excitations between Hartree-Fock molecular orbitals, to real-space exciton wavefunctions, expressed as linear combinations of particle-hole excitations between localized Wannier functions. The exciton wavefunction is a two-dimensional amplitude for the exciton center-of-mass coordinate, R, and the electron-hole separation (or relative coordinate), r, having an exact analogy to one-dimensional hydrogenlike wavefunctions. We describe the excitons by their appropriate quantum numbers, namely, the principle quantum number, n, associated with r and the center-of-mass pseudomomentum quantum number, j, associated with R. In addition, for models with particle-hole symmetry, such as the Pariser-Parr-Pople model, we emphasize the connection between particle-hole symmetry and particle-hole parity. The method is applied to the study of excitons in trans-polyacetylene and poly(para-phenylene).
The excited spin-triplet state of a charged exciton in quantum dots
NASA Astrophysics Data System (ADS)
Molas, M. R.; Nicolet, A. A. L.; Piętka, B.; Babiński, A.; Potemski, M.
2016-09-01
We report on spectroscopic studies of resonances related to ladder of states of a charged exciton in single GaAlAs/AlAs quantum dot structures. Polarization-resolved photoluminescence, photoluminescence excitation and photon-correlation measurements were performed at low (T = 4.2 K) temperature also in magnetic field applied in Faraday configuration. The investigated resonances are assigned to three different configurations of a positively charged exciton. Together with a singlet ground state and a conventional triplet state (involving an electron from the ground state electronic s-shell), an excited triplet state, which involved an electron from the excited electronic p-shell was identified in single dots. The appearance of an emission line related to the latter complex is due to a partially suppressed electron relaxation in the investigated dots. An analysis of this emission line allows us to scrupulously determine properties of the excited triplet state and compare them with those of the conventional triplet state. Both triplets exhibit similar patterns of anisotropic fine structure and Zeeman splitting, however their amplitudes significantly differ for those two states. Presented results emphasize the role of the symmetry of the electronic state on the properties of the triplet states of two holes + electron excitonic complex.
NASA Astrophysics Data System (ADS)
Slobodeniuk, A. O.; Basko, D. M.
2016-09-01
We perform a theoretical study of radiative decay of dark intravalley excitons in transition metal dichalcogenide monolayers. This decay necessarily involves an electronic spin flip. The intrinsic decay mechanism due to interband spin-flip dipole moment perpendicular to the monolayer plane, gives a rate about 100-1000 times smaller than that of bright excitons. However, we find that this mechanism also introduces an energy splitting due to a local field effect, and the whole oscillator strength is contained in the higher-energy component, while the lowest-energy state remains dark and needs an extrinsic spin-flip mechanism for the decay. Rashba effect due to a perpendicular electric field or a dielectric substrate, gives a negligible radiative decay rate (about 107 times slower than that of bright excitons). Spin flip due to Zeeman effect in a sufficiently strong in-plane magnetic field can give a decay rate comparable to that due to the intrinsic interband spin-flip dipole.
Renormalization group approach to the Fröhlich polaron model: application to impurity-BEC problem
Grusdt, F.; Shchadilova, Y. E.; Rubtsov, A. N.; Demler, E.
2015-01-01
When a mobile impurity interacts with a many-body system, such as a phonon bath, a polaron is formed. Despite the importance of the polaron problem for a wide range of physical systems, a unified theoretical description valid for arbitrary coupling strengths is still lacking. Here we develop a renormalization group approach for analyzing a paradigmatic model of polarons, the so-called Fröhlich model, and apply it to a problem of impurity atoms immersed in a Bose-Einstein condensate of ultra cold atoms. Polaron energies obtained by our method are in excellent agreement with recent diagrammatic Monte Carlo calculations for a wide range of interaction strengths. They are found to be logarithmically divergent with the ultra-violet cut-off, but physically meaningful regularized polaron energies are also presented. Moreover, we calculate the effective mass of polarons and find a smooth crossover from weak to strong coupling regimes. Possible experimental tests of our results in current experiments with ultra cold atoms are discussed. PMID:26183614
Experimental study of NIR absorption due to Nb4+ polarons in pure and Cr- or Ce-doped SBN crystals
NASA Astrophysics Data System (ADS)
Gao, Ming; Kapphan, S.; Porcher, S.; Pankrath, R.
1999-06-01
A broad absorption band around 0.72 eV, assigned to the absorption of Nb4+ polarons, is observed in strontium barium niobate (SBN) crystals (nominally pure or Cr- or Ce-doped) either under illumination at low temperature or after a previous reduction treatment. The absorption spectra of Nb4+ polarons at low temperature show considerable dichroism, which in reduced SBN crystals exists even far above room temperature. The peak position of the Nb4+ polaron absorption in reduced SBN crystals shifts to higher energies with decreasing temperature. The dependence on light intensity and temperature of the Nb4+ polaron absorption during the build-up process under illumination and the decay process after the illumination is switched off are investigated in detail. Compared with pure SBN, doping with Ce or Cr creates additional absorption bands in the visible (2.6 eV) and red (1.9 eV for Cr doping) spectral regions. Illumination in these absorption bands at low temperature gives rise to strong Nb4+ polaron absorption in the NIR (0.72 eV), giving evidence of the enhanced sensitivity even in the red spectral region for SBN:Cr. The light-induced charge transfer process and formation of Nb4+ polarons in SBN are briefly discussed.
Probing excitonic dark states in single-layer tungsten disulphide
NASA Astrophysics Data System (ADS)
Ye, Ziliang; Cao, Ting; O'Brien, Kevin; Zhu, Hanyu; Yin, Xiaobo; Wang, Yuan; Louie, Steven G.; Zhang, Xiang
2014-09-01
Transition metal dichalcogenide (TMDC) monolayers have recently emerged as an important class of two-dimensional semiconductors with potential for electronic and optoelectronic devices. Unlike semi-metallic graphene, layered TMDCs have a sizeable bandgap. More interestingly, when thinned down to a monolayer, TMDCs transform from indirect-bandgap to direct-bandgap semiconductors, exhibiting a number of intriguing optical phenomena such as valley-selective circular dichroism, doping-dependent charged excitons and strong photocurrent responses. However, the fundamental mechanism underlying such a strong light-matter interaction is still under intensive investigation. First-principles calculations have predicted a quasiparticle bandgap much larger than the measured optical gap, and an optical response dominated by excitonic effects. In particular, a recent study based on a GW plus Bethe-Salpeter equation (GW-BSE) approach, which employed many-body Green's-function methodology to address electron-electron and electron-hole interactions, theoretically predicted a diversity of strongly bound excitons. Here we report experimental evidence of a series of excitonic dark states in single-layer WS2 using two-photon excitation spectroscopy. In combination with GW-BSE theory, we prove that the excitons are of Wannier type, meaning that each exciton wavefunction extends over multiple unit cells, but with extraordinarily large binding energy (~0.7 electronvolts), leading to a quasiparticle bandgap of 2.7 electronvolts. These strongly bound exciton states are observed to be stable even at room temperature. We reveal an exciton series that deviates substantially from hydrogen models, with a novel energy dependence on the orbital angular momentum. These excitonic energy levels are experimentally found to be robust against environmental perturbations. The discovery of excitonic dark states and exceptionally large binding energy not only sheds light on the importance of many
Exciton Correlations in Intramolecular Singlet Fission
Sanders, Samuel N.; Kumarasamy, Elango; Pun, Andrew B.; ...
2016-05-16
We have synthesized a series of asymmetric pentacene-tetracene heterodimers with a variable-length conjugated bridge that undergo fast and efficient intramolecular singlet fission (iSF). These compounds have distinct singlet and triplet energies, which allow us to study the spatial dynamics of excitons during the iSF process, including the significant role of exciton correlations in promoting triplet pair generation and recombination. We demonstrate that the primary photoexcitations in conjugated dimers are delocalized singlets that enable fast and efficient iSF. However, in these asymmetric dimers, the singlet becomes more localized on the lower energy unit as the length of the bridge is increased,more » slowing down iSF relative to analogous symmetric dimers. We resolve the recombination kinetics of the inequivalent triplets produced via iSF, and find that they primarily decay via concerted processes. By identifying different decay channels, including delayed fluorescence via triplet-triplet annihilation, we can separate transient species corresponding to both correlated triplet pairs and uncorrelated triplets. Recombination of the triplet pair proceeds rapidly despite our experimental and theoretical demonstration that individual triplets are highly localized and unable to be transported across the conjugated linker. In this class of compounds, the rate of formation and yield of uncorrelated triplets increases with bridge length. Overall, these constrained, asymmetric systems provide a unique platform to isolate and study transient species essential for singlet fission, which are otherwise difficult to observe in symmetric dimers or condensed phases.« less
Exciton Correlations in Intramolecular Singlet Fission
Sanders, Samuel N.; Kumarasamy, Elango; Pun, Andrew B.; Appavoo, Kannatassen; Steigerwald, Michael L.; Campos, Luis M.; Sfeir, Matthew Y.
2016-05-16
We have synthesized a series of asymmetric pentacene-tetracene heterodimers with a variable-length conjugated bridge that undergo fast and efficient intramolecular singlet fission (iSF). These compounds have distinct singlet and triplet energies, which allow us to study the spatial dynamics of excitons during the iSF process, including the significant role of exciton correlations in promoting triplet pair generation and recombination. We demonstrate that the primary photoexcitations in conjugated dimers are delocalized singlets that enable fast and efficient iSF. However, in these asymmetric dimers, the singlet becomes more localized on the lower energy unit as the length of the bridge is increased, slowing down iSF relative to analogous symmetric dimers. We resolve the recombination kinetics of the inequivalent triplets produced via iSF, and find that they primarily decay via concerted processes. By identifying different decay channels, including delayed fluorescence via triplet-triplet annihilation, we can separate transient species corresponding to both correlated triplet pairs and uncorrelated triplets. Recombination of the triplet pair proceeds rapidly despite our experimental and theoretical demonstration that individual triplets are highly localized and unable to be transported across the conjugated linker. In this class of compounds, the rate of formation and yield of uncorrelated triplets increases with bridge length. Overall, these constrained, asymmetric systems provide a unique platform to isolate and study transient species essential for singlet fission, which are otherwise difficult to observe in symmetric dimers or condensed phases.
Exciton Dynamics in Semiconducting Carbon Nanotubes
Graham, Matt; Chmeliov, Javgenij; Ma, Yingzhong; Shinohara, Nori; Green, Alexander A.; Hersam, Mark C.; Valkunas, Leonas; Fleming, Graham
2010-01-01
We report femtosecond transient absorption spectroscopic study on the (6, 5) single-walled carbon nanotubes and the (7, 5) inner tubes of a dominant double-walled carbon nanotube species. We found that the dynamics of exciton relaxation probed at the first transition-allowed state (E11) of a given tube type exhibits a markedly slower decay when the second transition-allowed state (E22) is excited than that measured by exciting its first transition-allowed state (E11). A linear intensity dependence of the maximal amplitude of the transient absorption signal is found for the E22 excitation, whereas the corresponding amplitude scales linearly with the square root of the E11 excitation intensity. Theoretical modeling of these experimental findings was performed by developing a continuum model and a stochastic model with explicit consideration of the annihilation of coherent excitons. Our detailed numerical simulations show that both models can reproduce reasonably well the initial portion of decay kinetics measured upon the E22 and E11 excitation of the chosen tube species, but the stochastic model gives qualitatively better agreement with the intensity dependence observed experimentally than those obtained with the continuum model.
Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS_{2} and MoS_{2} to 65 Tesla
Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T.; Kono, Junichiro; Crooker, Scott A.
2016-02-09
In bulk and quantum-confined semiconductors, magneto-optical studies have historically played an essential role in determining the fundamental parameters of excitons (size, binding energy, spin, dimensionality and so on). Here we report low-temperature polarized reflection spectroscopy of atomically thin WS_{2} and MoS_{2} in high magnetic fields to 65 T. Both the A and B excitons exhibit similar Zeeman splittings of approximately –230 μeV T–1 (g-factor ≃–4), thereby quantifying the valley Zeeman effect in monolayer transition-metal disulphides. Crucially, these large fields also allow observation of the small quadratic diamagnetic shifts of both A and B excitons in monolayer WS_{2}, from which radii of ~1.53 and ~1.16 nm are calculated. Further, when analysed within a model of non-local dielectric screening, these diamagnetic shifts also constrain estimates of the A and B exciton binding energies (410 and 470 meV, respectively, using a reduced A exciton mass of 0.16 times the free electron mass). Lastly, these results highlight the utility of high magnetic fields for understanding new two-dimensional materials.
Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla.
Stier, Andreas V; McCreary, Kathleen M; Jonker, Berend T; Kono, Junichiro; Crooker, Scott A
2016-02-09
In bulk and quantum-confined semiconductors, magneto-optical studies have historically played an essential role in determining the fundamental parameters of excitons (size, binding energy, spin, dimensionality and so on). Here we report low-temperature polarized reflection spectroscopy of atomically thin WS2 and MoS2 in high magnetic fields to 65 T. Both the A and B excitons exhibit similar Zeeman splittings of approximately -230 μeV T(-1) (g-factor ≃-4), thereby quantifying the valley Zeeman effect in monolayer transition-metal disulphides. Crucially, these large fields also allow observation of the small quadratic diamagnetic shifts of both A and B excitons in monolayer WS2, from which radii of ∼1.53 and ∼1.16 nm are calculated. Further, when analysed within a model of non-local dielectric screening, these diamagnetic shifts also constrain estimates of the A and B exciton binding energies (410 and 470 meV, respectively, using a reduced A exciton mass of 0.16 times the free electron mass). These results highlight the utility of high magnetic fields for understanding new two-dimensional materials.
Electron small polarons and their transport in bismuth vanadate: a first principles study.
Kweon, Kyoung E; Hwang, Gyeong S; Kim, Jinhan; Kim, Sungjin; Kim, SeongMin
2015-01-07
Relatively low electron mobility has been thought to be a key factor that limits the overall photocatalytic performance of BiVO4, but the behavior of electrons has not been fully elucidated. We examine electron localization and transport in BiVO4 using hybrid density functional theory calculations. An excess electron is found to remain largely localized on one V atom. The predicted hopping barrier for the small polaron is 0.35 eV (with inclusion of 15% Hartree-Fock exchange), and tends to increase almost linearly with lattice constant associated with pressure and/or temperature changes. We also examine the interaction between polarons, and discuss the possible concentration-dependence of electron mobility in BiVO4.
Rashba Effect on the Bound Polaron in an Asymmetric Quantum Dot
NASA Astrophysics Data System (ADS)
Shan, Shu-Ping; Chen, Shi-Hua; Xiao, Jing-Lin
2014-07-01
By using LLP variational method, the Rashba effect on the bound polaron in an asymmetric quantum dot is investigated and the expression of the bound polaron ground state energy is derived. Considering different Coulomb bound potentials, we discuss the relations between the ground state energy and the electron-phonon coupling strength, the wave vector, the transverse effective confinement length and the longitudsinal effective confinement length, respectively. The results show that the ground state energy is a decreasing function of the Coulomb bound potential, the electron-phonon coupling strength, the transverse effective confinement length and the longitudinal effective confinement length. On the contrary, it is an increasing function of the wave vector. Due to the Rashba effect, the ground state energy splits into two branches.
Study of strong-coupling impurity bound polaron in a quantum pseudodot
NASA Astrophysics Data System (ADS)
Khordad, R.
2015-01-01
In the present work, we have studied the first internal excited state energy and transition frequency of strong-coupling impurity bound polaron in a quantum pseudodot using the well-known Lee-Low-Pines (LLP) unitary transformation method. We show the effect of Coulomb bound potential, electron-phonon (e-p) coupling strength, the quantum dot radius and potential height on first internal excited state energy and the transition frequency of the impurity bound polaron. According to the results, it is found that the first internal excited state energy is decreased with increasing quantum dot radius. Also, this energy is increased with enhancing potential height. The transition frequency is increased with increasing the e-p coupling strength. Also, the first internal excited state energy is increased with decreasing the e-p coupling strength. The transition frequency is enhanced with increasing the Coulomb bound potential.
Fermi polaron in two dimensions: Importance of the two-body bound state
Klawunn, Michael; Recati, Alessio
2011-09-15
We investigate a single impurity interacting with a free two-dimensional atomic Fermi gas. The interaction between the impurity and the gas is characterized by an arbitrary attractive short-range potential, which, in two dimensions, always admits a two-particle bound state. We provide analytical expressions for the energy and the effective mass of the dressed impurity by including the two-body bound state, which is crucial for strong interactions, in the integral equation for the effective interaction. Using the same method, we also give the results for the polaron parameters in one and three dimensions and find good agreement with previous results. Thus, our relations can be used as a simple way to estimate the polaron parameters once the two-body bound state of the interaction potential is known.
Spin-polaron nature of fermion quasiparticles and their d-wave pairing in cuprate superconductors
NASA Astrophysics Data System (ADS)
Val'kov, V. V.; Dzebisashvili, D. M.; Barabanov, A. F.
2016-11-01
In the framework of the spin-fermion model, to which the Emery model is reduced in the limit of strong electron correlations, it is shown that the fermion quasiparticles in cuprate high- T c superconductors (HTSCs) arise under a strong effect of exchange coupling between oxygen holes and spins of copper ions. This underlies the spin-polaron nature of fermion quasiparticles in cuprate HTSCs. The Cooper instability with respect to the d-wave symmetry of the order parameter is revealed for an ensemble of such quasiparticles. For the normal phase, the spin-polaron concept allows us to reproduce the fine details in the evolution of the Fermi surface with the changes in the doping level x observed in experiment for La2-xSrxCuO4. The calculated T-x phase diagram correlates well with the available experimental data for cuprate HTSCs.
Tunable breakdown of the polaron picture for mobile impurities in a topological semimetal
NASA Astrophysics Data System (ADS)
Caracanhas, M. A.; Pereira, R. G.
2016-12-01
Mobile impurities in cold atomic gases constitute a new platform for investigating polaron physics. Here we show that when impurity atoms interact with a two-dimensional Fermi gas with quadratic band touching, the polaron picture may either hold or break down depending on the particle-hole asymmetry of the band structure. If the hole band has a smaller effective mass than the particle band, the quasiparticle is stable and its diffusion coefficient varies with temperature as D (T ) ∝ln2T . If the hole band has larger mass, the quasiparticle weight vanishes at low energies due to an emergent orthogonality catastrophe. In this case we map the problem onto a set of one-dimensional channels and use conformal field theory techniques to obtain D (T ) ∝Tν with an interaction-dependent exponent ν . The different regimes can be detected in the nonequilibrium expansion dynamics of an initially confined impurity.
Polaron Coherence Condensation As the Mechanism for Colossal Magnetoresistance in Layered Manganites
Mannella, N.; Yang, W.L.; Tanaka, K.; Zhou, X.J.; Zheng, H.; Mitchell, J.F.; Zaanen, J.; Devereaux, T.P.; Nagaosa, N.; Hussain, Z.; Shen, Z.-X.; /SLAC
2007-11-20
Angle-resolved photoemission spectroscopy data for the bilayer manganite La{sub 1.2}Sr{sub 1.8}Mn{sub 2}O{sub 7} show that, upon lowering the temperature below the Curie point, a coherent polaronic metallic groundstate emerges very rapidly with well defined quasiparticles which track remarkably well the electrical conductivity, consistent with macroscopic transport properties. Our data suggest that the mechanism leading to the insulator-to-metal transition in La{sub 1.2}Sr{sub 1.8}Mn{sub 2}O{sub 7} can be regarded as a polaron coherence condensation process acting in concert with the Double Exchange interaction.
Neukirch, Amanda J.; Nie, Wanyi; Blancon, Jean-Christophe; ...
2016-05-25
Solution-processed organometallic perovskites have rapidly developed into a top candidate for the active layer of photovoltaic devices. In spite of the remarkable progress associated with perovskite materials, many questions about the fundamental photophysical processes taking place in these devices, remain open. High on the list of unexplained phenomena are very modest mobilities despite low charge carrier effective masses. Moreover, experiments elucidate unique degradation of photocurrent affecting stable operation of perovskite solar cells. These puzzles suggest that, while ionic hybrid perovskite devices may have efficiencies on par with conventional Si and GaAs devices, they exhibit more complicated charge transport phenomena. Wemore » report the results from an in-depth computational study of small polaron formation, electronic structure, charge density, and reorganization energies using both periodic boundary conditions and isolated structures. Using the hybrid density functional theory, we found that volumetric strain in a CsPbI3 cluster creates a polaron with binding energy of around 300 and 900 meV for holes and electrons, respectively. In the MAPbI3 (MA = CH3NH3) cluster, both volumetric strain and MA reorientation effects lead to larger binding energies at around 600 and 1300 meV for holes and electrons, respectively. Such large reorganization energies suggest appearance of small polarons in organometallic perovskite materials. Furthermore, the fact that both volumetric lattice strain and MA molecular rotational degrees of freedom can cooperate to create and stabilize polarons indicates that in order to mitigate this problem, formamidinium (FA = HC(NH2)2) and cesium (Cs) based crystals and alloys, are potentially better materials for solar cell and other optoelectronic applications.« less
Neukirch, Amanda J.; Nie, Wanyi; Blancon, Jean-Christophe; Appavoo, Kannatassen; Tsai, Hsinhan; Sfeir, Matthew Y.; Katan, Claudine; Pedesseau, Laurent; Even, Jacky; Crochet, Jared J.; Gupta, Gautam; Mohite, Aditya D.; Tretiak, Sergei
2016-05-25
Solution-processed organometallic perovskites have rapidly developed into a top candidate for the active layer of photovoltaic devices. In spite of the remarkable progress associated with perovskite materials, many questions about the fundamental photophysical processes taking place in these devices, remain open. High on the list of unexplained phenomena are very modest mobilities despite low charge carrier effective masses. Moreover, experiments elucidate unique degradation of photocurrent affecting stable operation of perovskite solar cells. These puzzles suggest that, while ionic hybrid perovskite devices may have efficiencies on par with conventional Si and GaAs devices, they exhibit more complicated charge transport phenomena. We report the results from an in-depth computational study of small polaron formation, electronic structure, charge density, and reorganization energies using both periodic boundary conditions and isolated structures. Using the hybrid density functional theory, we found that volumetric strain in a CsPbI_{3} cluster creates a polaron with binding energy of around 300 and 900 meV for holes and electrons, respectively. In the MAPbI_{3} (MA = CH_{3}NH_{3}) cluster, both volumetric strain and MA reorientation effects lead to larger binding energies at around 600 and 1300 meV for holes and electrons, respectively. Such large reorganization energies suggest appearance of small polarons in organometallic perovskite materials. Furthermore, the fact that both volumetric lattice strain and MA molecular rotational degrees of freedom can cooperate to create and stabilize polarons indicates that in order to mitigate this problem, formamidinium (FA = HC(NH_{2})_{2}) and cesium (Cs) based crystals and alloys, are potentially better materials for solar cell and other optoelectronic applications.
Polaronic contributions to oxidation and hole conductivity in acceptor-doped BaZrO3
NASA Astrophysics Data System (ADS)
Lindman, Anders; Erhart, Paul; Wahnström, Göran
2016-08-01
Acceptor-doped perovskite oxides like BaZrO3 are showing great potential as materials for renewable energy technologies where hydrogen acts an energy carrier, such as solid oxide fuel cells and hydrogen separation membranes. While ionic transport in these materials has been investigated intensively, the electronic counterpart has received much less attention and further exploration in this field is required. Here, we use density functional theory (DFT) to study hole polarons and their impact on hole conductivity in Y-doped BaZrO3. Three different approaches have been used to remedy the self-interaction error of local and semilocal exchange-correlation functionals: DFT +U , pSIC-DFT, and hybrid functionals. Self-trapped holes are found to be energetically favorable by about -0.1 eV and the presence of yttrium results in further stabilization. Polaron migration is predicted to occur through intraoctahedral transfer and polaron rotational processes, which are associated with adiabatic barriers of about 0.1 eV. However, the rather small energies associated with polaron formation and migration suggest that the hole becomes delocalized and bandlike at elevated temperatures. These results together with an endothermic oxidation reaction [A. Lindman, P. Erhart, and G. Wahnström, Phys. Rev. B 91, 245114 (2015), 10.1103/PhysRevB.91.245114] yield a picture that is consistent with experimental data for the hole conductivity. The results we present here provide new insight into hole transport in acceptor-doped BaZrO3 and similar materials, which will be of value in the future development of sustainable technologies.
Polaronic atom-trimer continuity in three-component Fermi gases.
Nishida, Yusuke
2015-03-20
Recently it has been proposed that three-component Fermi gases may exhibit a new type of crossover physics in which an unpaired Fermi sea of atoms smoothly evolves into that of trimers in addition to the ordinary BCS-BEC crossover of condensed pairs. Here we study its corresponding polaron problem in which a single impurity atom of one component interacts with condensed pairs of the other two components with equal populations. By developing a variational approach in the vicinity of a narrow Feshbach resonance, we show that the impurity atom smoothly changes its character from atom to trimer with increasing the attraction and eventually there is a sharp transition to dimer. The emergent polaronic atom-trimer continuity can be probed in ultracold atoms experiments by measuring the impurity spectral function. Our novel crossover wave function properly incorporating the polaronic atom-trimer continuity will provide a useful basis to further investigate the phase diagram of three-component Fermi gases in more general situations.
Small polaron characteristics of the OH center in TiO2
NASA Astrophysics Data System (ADS)
Fowler, W. Beall
2013-03-01
Most insulating crystals have nearly-free-electron conduction bands and corresponding conduction properties, with the effective mass increased slightly by large-polaron effects. In TiO2, the lowest conduction bands contain considerable admixture of Ti 3d states. In this case the conduction electrons become localized, or self-trapped, into small-polaron states, and their conduction properties differ considerably from the usual case. EPR experiments by Halliburton et al. have shown that this self-trapping is also present in association with point defects, namely substitutional F and interstitial H (which forms a bond with a lattice O). In each case the spin of the unpaired electron is localized on a nearest neighbor Ti. Infrared absorption experiments as a function of temperature on the OH center by Bekisli et al. have resolved apparent inconsistencies in the model used to fit earlier IR data. Through detailed analysis they have interpreted their results in terms of a small polaron model which involves several configurations corresponding to the localization of the OH electron on different Ti sites, each of which yields an IR line of slightly different frequency. These conclusions are supported by theoretical results in the literature and by our calculations using the CRYSTAL06 code with a hybridized DFT Hamiltonian. This work was done in collaboration with Figen Bekisli and Michael Stavola, and was supported by NSF Grant No. DMR 1160756.
Mapping polarons in polymer FETs by charge modulation microscopy in the mid-infrared
Chin, Xin Yu; Yin, Jun; Wang, Zilong; Caironi, Mario; Soci, Cesare
2014-01-01
We implemented spatial mapping of charge carrier density in the channel of a conventional polymer Field-Effect Transistor (FET) by mid-infrared Charge Modulation Spectroscopy (CMS). CMS spectra are recorded with a high sensitivity confocal Fourier Transform Infra-Red (FTIR) microscope by probing electroinduced Infra-Red Active Vibrational (IRAV) modes and low-energy polaron bands in the spectral region 680–4000 cm−1. Thanks to the high specificity and strong oscillator strength of these modes, charge-induced reflectance measurements allow quantitative estimation of charge carrier densities within the FET channel, without the need for amplitude or phase modulation. This is illustrated by identifying the contribution of intrinsic and electrostatically induced polarons to conduction, and by mapping the polaron spatial distribution in a P3HT (Poly(3-hexylthiophene-2,5-diyl)) FET channel under different drain-source bias conditions. This work demonstrates the potential of mid-infrared charge modulation microscopy to characterize carrier injection and transport in semiconducting polymer materials. PMID:24406635
DFT +U Modeling of Hole Polarons in Organic Lead Halide Perovskites
NASA Astrophysics Data System (ADS)
Welch, Eric; Erhart, Paul; Scolfaro, Luisa; Zakhidov, Alex
Due to the ever present drive towards improved efficiencies in solar cell technology, new and improved materials are emerging rapidly. Organic halide perovskites are a promising prospect, yet a fundamental understanding of the organic perovskite structure and electronic properties is missing. Particularly, explanations of certain physical phenomena, specifically a low recombination rate and high mobility of charge carriers still remain controversial. We theoretically investigate possible formation of hole polarons adopting methodology used for oxide perovskites. The perovskite studied here is the ABX3structure, with A being an organic cation, B lead and C a halogen; the combinations studied allow for A1,xA2 , 1 - xBX1,xX2 , 3 - xwhere the alloy convention is used to show mixtures of the organic cations and/or the halogens. Two organic cations, methylammonium and formamidinium, and three halogens, iodine, chlorine and bromine are studied. Electronic structures and polaron behavior is studied through first principle density functional theory (DFT) calculations using the Vienna Ab Initio Simulation Package (VASP). Local density approximation (LDA) pseudopotentials are used and a +U Hubbard correction of 8 eV is added; this method was shown to work with oxide perovskites. It is shown that a localized state is realized with the Hubbard correction in systems with an electron removed, residing in the band gap of each different structure. Thus, hole polarons are expected to be seen in these perovskites.
High-density two-dimensional small polaron gas in a delta-doped Mott insulator.
Ouellette, Daniel G; Moetakef, Pouya; Cain, Tyler A; Zhang, Jack Y; Stemmer, Susanne; Emin, David; Allen, S James
2013-11-21
Heterointerfaces in complex oxide systems open new arenas in which to test models of strongly correlated material, explore the role of dimensionality in metal-insulator-transitions (MITs) and small polaron formation. Close to the quantum critical point Mott MITs depend on band filling controlled by random disordered substitutional doping. Delta-doped Mott insulators are potentially free of random disorder and introduce a new arena in which to explore the effect of electron correlations and dimensionality. Epitaxial films of the prototypical Mott insulator GdTiO3 are delta-doped by substituting a single (GdO)(+1) plane with a monolayer of charge neutral SrO to produce a two-dimensional system with high planar doping density. Unlike metallic SrTiO3 quantum wells in GdTiO3 the single SrO delta-doped layer exhibits thermally activated DC and optical conductivity that agree in a quantitative manner with predictions of small polaron transport but with an extremely high two-dimensional density of polarons, ~7 × 10(14) cm(-2).
High-density Two-Dimensional Small Polaron Gas in a Delta-Doped Mott Insulator
Ouellette, Daniel G.; Moetakef, Pouya; Cain, Tyler A.; Zhang, Jack Y.; Stemmer, Susanne; Emin, David; Allen, S. James
2013-01-01
Heterointerfaces in complex oxide systems open new arenas in which to test models of strongly correlated material, explore the role of dimensionality in metal-insulator-transitions (MITs) and small polaron formation. Close to the quantum critical point Mott MITs depend on band filling controlled by random disordered substitutional doping. Delta-doped Mott insulators are potentially free of random disorder and introduce a new arena in which to explore the effect of electron correlations and dimensionality. Epitaxial films of the prototypical Mott insulator GdTiO3 are delta-doped by substituting a single (GdO)+1 plane with a monolayer of charge neutral SrO to produce a two-dimensional system with high planar doping density. Unlike metallic SrTiO3 quantum wells in GdTiO3 the single SrO delta-doped layer exhibits thermally activated DC and optical conductivity that agree in a quantitative manner with predictions of small polaron transport but with an extremely high two-dimensional density of polarons, ~7 × 1014 cm−2. PMID:24257578
Mapping polaronic states and lithiation gradients in individual V2O5 nanowires
NASA Astrophysics Data System (ADS)
de Jesus, Luis R.; Horrocks, Gregory A.; Liang, Yufeng; Parija, Abhishek; Jaye, Cherno; Wangoh, Linda; Wang, Jian; Fischer, Daniel A.; Piper, Louis F. J.; Prendergast, David; Banerjee, Sarbajit
2016-06-01
The rapid insertion and extraction of Li ions from a cathode material is imperative for the functioning of a Li-ion battery. In many cathode materials such as LiCoO2, lithiation proceeds through solid-solution formation, whereas in other materials such as LiFePO4 lithiation/delithiation is accompanied by a phase transition between Li-rich and Li-poor phases. We demonstrate using scanning transmission X-ray microscopy (STXM) that in individual nanowires of layered V2O5, lithiation gradients observed on Li-ion intercalation arise from electron localization and local structural polarization. Electrons localized on the V2O5 framework couple to local structural distortions, giving rise to small polarons that serves as a bottleneck for further Li-ion insertion. The stabilization of this polaron impedes equilibration of charge density across the nanowire and gives rise to distinctive domains. The enhancement in charge/discharge rates for this material on nanostructuring can be attributed to circumventing challenges with charge transport from polaron formation.
Path-dependent initialization of a single quantum dot exciton spin in a nanophotonic waveguide
NASA Astrophysics Data System (ADS)
Coles, R. J.; Price, D. M.; Royall, B.; Clarke, E.; Skolnick, M. S.; Fox, A. M.; Makhonin, M. N.
2017-03-01
We demonstrate a scheme for in-plane initialization of a single exciton spin in an InGaAs quantum dot (QD) coupled to a GaAs nanobeam waveguide. The chiral coupling of the QD and the optical mode of the nanobeam enables spin initialization fidelity approaching unity in magnetic field B =1 T and >0.9 without the field. We further show that this in-plane excitation scheme is independent of the incident excitation laser polarization and depends solely on the excitation direction. This scheme provides a robust in-plane spin excitation basis for a photon-mediated spin network for quantum information applications.
Novel exciton systems in 2D TMD monolayers and heterobilayers
NASA Astrophysics Data System (ADS)
Yu, Hongyi
In this talk, two exciton systems in transition metal dichalcogenides (TMDs) monolayer and heterobilayer will be discussed. In TMD monolayers, the strong e-h Coulomb exchange interaction splits the exciton and trion dispersions into two branches with zero and finite gap, respectively. Each branch is a center-of-mass wave vector dependent coherent superposition of the two valleys, which leads to a valley-orbit coupling and possibly a trion valley Hall effect. The exchange interaction also eliminates the linear polarization of the negative trion PL emission. In TMD heterobilayers with a type-II band alignment, the low energy exciton has an interlayer configuration with the e and h localized in opposite layers. Because of the inevitable twist or/and lattice mismatch between the two layers, the bright interlayer excitons are located at finite center-of-mass velocities with a six-fold degeneracy. The corresponding photon emission is elliptically polarized, with the major axis locked to the direction of exciton velocity, and helicity determined by the valley indices of the e and h. Some experimental results on the interlayer excitons in the WSe2-MoSe2 heterobilayers will also be presented. The interlayer exciton exhibits a long lifetime as well as a long depolarization time, which facilitate the observation of a PL polarization ring pattern due to the valley dependent exciton-exciton interaction induced expansion. The works were supported by the Research Grant Council of Hong Kong (HKU17305914P, HKU705513P), the Croucher Foundation, and the HKU OYRA and ROP.
Hot exciton cooling and multiple exciton generation in PbSe quantum dots.
Kumar, Manoj; Vezzoli, Stefano; Wang, Zilong; Chaudhary, Varun; Ramanujan, Raju V; Gurzadyan, Gagik G; Bruno, Annalisa; Soci, Cesare
2016-11-16
Multiple exciton generation (MEG) is a promising process to improve the power conversion efficiency of solar cells. PbSe quantum dots (QDs) have shown reasonably high MEG quantum yield (QY), although the photon energy threshold for this process is still under debate. One of the reasons for this inconsistency is the complicated competition of MEG and hot exciton cooling, especially at higher excited states. Here, we investigate MEG QY and the origin of the photon energy threshold for MEG in PbSe QDs of three different sizes by studying the transient absorption (TA) spectra, both at the band gap (near infrared, NIR) and far from the band gap energy (visible range). The comparison of visible TA spectra and dynamics for different pump wavelengths, below, around and above the MEG threshold, provides evidence of the role of the Σ transition in slowing down the exciton cooling process that can help MEG to take over the phonon relaxation process. The universality of this behavior is confirmed by studying QDs of three different sizes. Moreover, our results suggest that MEG QY can be determined by pump-probe experiments probed above the band gap.
Ubiquity of Exciton Localization in Cryogenic Carbon Nanotubes
2016-01-01
We present photoluminescence studies of individual semiconducting single-wall carbon nanotubes at room and cryogenic temperatures. From the analysis of spatial and spectral features of nanotube photoluminescence, we identify characteristic signatures of unintentional exciton localization. Moreover, we quantify the energy scale of exciton localization potentials as ranging from a few to a few tens of millielectronvolts and stemming from both environmental disorder and shallow covalent side-wall defects. Our results establish disorder-induced crossover from the diffusive to the localized regime of nanotube excitons at cryogenic temperatures as a ubiquitous phenomenon in micelle-encapsulated and as-grown carbon nanotubes. PMID:27105355
Quantized Vortices and Four-Component Superfluidity of Semiconductor Excitons
NASA Astrophysics Data System (ADS)
Anankine, Romain; Beian, Mussie; Dang, Suzanne; Alloing, Mathieu; Cambril, Edmond; Merghem, Kamel; Carbonell, Carmen Gomez; Lemaître, Aristide; Dubin, François
2017-03-01
We study spatially indirect excitons of GaAs quantum wells, confined in a 10 μ m electrostatic trap. Below a critical temperature of about 1 K, we detect macroscopic spatial coherence and quantized vortices in the weak photoluminescence emitted from the trap. These quantum signatures are restricted to a narrow range of density, in a dilute regime. They manifest the formation of a four-component superfluid, made by a low population of optically bright excitons coherently coupled to a dominant fraction of optically dark excitons.
Excitonic AND Logic Gates on DNA Brick Nanobreadboards
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
Excitons and the lifetime of organic semiconductor devices
Forrest, Stephen R.
2015-01-01
While excitons are responsible for the many beneficial optical properties of organic semiconductors, their non-radiative recombination within the material can result in material degradation due to the dumping of energy onto localized molecular bonds. This presents a challenge in developing strategies to exploit the benefits of excitons without negatively impacting the device operational stability. Here, we will briefly review the fundamental mechanisms leading to excitonic energy-driven device ageing in two example devices: blue emitting electrophosphorescent organic light emitting devices (PHOLEDs) and organic photovoltaic (OPV) cells. We describe strategies used to minimize or even eliminate this fundamental device degradation pathway. PMID:25987572
Excitons and the lifetime of organic semiconductor devices.
Forrest, Stephen R
2015-06-28
While excitons are responsible for the many beneficial optical properties of organic semiconductors, their non-radiative recombination within the material can result in material degradation due to the dumping of energy onto localized molecular bonds. This presents a challenge in developing strategies to exploit the benefits of excitons without negatively impacting the device operational stability. Here, we will briefly review the fundamental mechanisms leading to excitonic energy-driven device ageing in two example devices: blue emitting electrophosphorescent organic light emitting devices (PHOLEDs) and organic photovoltaic (OPV) cells. We describe strategies used to minimize or even eliminate this fundamental device degradation pathway.
Ubiquity of Exciton Localization in Cryogenic Carbon Nanotubes.
Hofmann, Matthias S; Noé, Jonathan; Kneer, Alexander; Crochet, Jared J; Högele, Alexander
2016-05-11
We present photoluminescence studies of individual semiconducting single-wall carbon nanotubes at room and cryogenic temperatures. From the analysis of spatial and spectral features of nanotube photoluminescence, we identify characteristic signatures of unintentional exciton localization. Moreover, we quantify the energy scale of exciton localization potentials as ranging from a few to a few tens of millielectronvolts and stemming from both environmental disorder and shallow covalent side-wall defects. Our results establish disorder-induced crossover from the diffusive to the localized regime of nanotube excitons at cryogenic temperatures as a ubiquitous phenomenon in micelle-encapsulated and as-grown carbon nanotubes.
Ultrafast excitonic room temperature nonlinearity in neutron irradiated quantum wells
Ten, S.; Williams, J.G.; Guerreiro, P.T.; Khitrova, G.; Peyghambarian, N.
1997-01-01
Sharp room temperature exciton features and complete recovery of the excitonic absorption with 21 ps time constant are demonstrated in neutron irradiated (Ga,Al)As/GaAs multiple quantum wells. Carrier lifetime reduction is consistent with the EL2 midgap defect which is efficiently generated by fast neutrons. Influence of gamma rays accompanying neutron irradiation is discussed. Neutron irradiation provides a straightforward way to control carrier lifetime in semiconductor heterostructures with minor deterioration of their excitonic properties. {copyright} {ital 1997 American Institute of Physics.}
Excitonic AND Logic Gates on DNA Brick Nanobreadboards.
Cannon, Brittany L; Kellis, Donald L; Davis, Paul H; Lee, Jeunghoon; Kuang, Wan; Hughes, William L; Graugnard, Elton; Yurke, Bernard; Knowlton, William B
2015-03-18
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.
Exciton coupling of surface complexes on a nanocrystal surface.
Xu, Xiangxing; Ji, Jianwei; Wang, Guan; You, Xiaozeng
2014-08-25
Exciton coupling may arise when chromophores are brought into close spatial proximity. Herein the intra-nanocrystal exciton coupling of the surface complexes formed by coordination of 8-hydroxyquinoline to ZnS nanocrystals (NCs) is reported. It is studied by absorption, photoluminescence (PL), PL excitation (PLE), and PL lifetime measurements. The exciton coupling of the surface complexes tunes the PL color and broadens the absorption and PLE windows of the NCs, and thus is a potential strategy for improving the light-harvesting efficiency of NC solar cells and photocatalysts.
Role of phonons in Josephson oscillations of excitonic and polaritonic condensates
Magnusson, E. B.; Flayac, H.; Malpuech, G.; Shelykh, I. A.
2010-11-15
We analyze theoretically the role of the exciton-phonon interactions in phenomena related to the Josephson effect between two spatially separated exciton and exciton-polariton condensates. We consider the role of the dephasing introduced by phonons in such phenomena as Josephson tunneling, self-trapping and spontaneous polarization separation. In the regime of cw pumping we find a remarkable bistability effect arising from exciton-exciton interactions as well as regimes of self-sustained regular and chaotic oscillations.
Dopant-Catalyzed Singlet Exciton Fission.
Snamina, Mateusz; Petelenz, Piotr
2017-01-04
In acene-based molecular crystals, singlet exciton fission occurs through superexchange mediated by two virtual charge-transfer states. Hence, it is sensitive to their energies, which depend on the local environment. The crucial point is the balance between the charge-quadrupole interactions within the pair of molecules directly involved in the process and those with the surrounding crystal matrix, which are governed by local symmetry and may be influenced by breaking this symmetry. This happens, for example, in the vicinity of a vacancy or an impurity and in the latter case is complemented by polarization energy and potentially by dipolar contributions. Our model calculations indicate that the superexchange coupling is sensitive enough to these factors to enable fission to be catalyzed by judiciously designed dopant molecules. In favorable cases, dipolar dopants are expected to increase the fission rate by an order of magnitude.
Bruggemann, B; May, V
2004-02-01
Using the multiexciton density matrix theory of excitation energy transfer in chromophore complexes developed in a foregoing paper [J. Chem. Phys. 118, 746 (2003)], the computation of ultrafast transient absorption spectra is presented. Beside static disorder and standard mechanisms of excitation energy dissipation the theory incorporates exciton exciton annihilation (EEA) processes. To elucidate signatures of EEA in intensity dependent transient absorption data the approach is applied to the B850 ring of the LH2 found in rhodobacter sphaeroides. As main indications for two-exciton population and resulting EEA we found (i) a weakening of the dominant single-exciton bleaching structure in the transient absorption, and (ii) an intermediate suppression of long-wavelength and short-wavelength shoulders around the bleaching structure. The suppression is caused by stimulated emission from the two-exciton to the one-exciton state and the return of the shoulders follows from a depletion of two-exciton population according to EEA. The EEA-signature survives as a short-wavelength shoulder in the transient absorption if orientational and energetic disorder are taken into account. Therefore, the observation of the EEA-signatures should be possible when doing frequency resolved transient absorption experiments with a sufficiently strongly varying pump-pulse intensity.
Control of Exciton Photon Coupling in Nano-structures
NASA Astrophysics Data System (ADS)
Liu, Xiaoze
In this thesis, we study the interaction of excitons with photons and plasmons and methods to control and enhance this interaction. This study is categorized in three parts: light-matter interaction in microcavity structures, direct dipole-dipole interactions, and plasmon-exciton interaction in metal-semiconductor systems. In the microcavity structures, the light-matter interactions become significant when the excitonic energy is in resonance with microcavity photons. New hybrid quantum states named polariton states will be formed if the strong coupling regime is achieved, where the interaction rate is faster than the average decay rate of the excitons and photons. Polaritons have been investigated in zinc oxide (ZnO) nanoparticles based microcavity at room temperature and stimulated emission of the polaritons has also been observed with a low optical pump threshold. Exictons in organic semiconductors (modeled as Frenkel excitons) are tightly bound to molecular sites, and differ considerably from loosely bound hydrogen atom-like inorganic excitons (modeled as Wannier-Mott excitons). This fundamental difference results in distinct optoelectronic properties. Not only strongly coupled to Wannier-Mott excitons in ZnO, the microcavity photons have also been observed to be simultaneously coupled to Frenkel excitons in 3,4,7,8-naphthalene tetracarboxylic dianhydride (NTCDA). The photons here act like a glue combining Wannier-Mott and Frenkel excitons into new hybrid polaritons taking the best from both constituents. Two-dimensional (2D) excitons in monolayer transition metal dichalcogenides (TMDs) have emerged as a new and fascinating type of Wannier-Mott-like excitons due to direct bandgap transition, huge oscillator strength and large binding energy. Monolayer molybdenum disulfide (MoS2) has been incorporated into the microcavity structure and 2D exciton-polaritons have been observed for the first time with directional emission in the strong coupling regime. Valley
Kirm, M.; Nagirnyi, V.; Feldbach, E.; De Grazia, M.; Carre, B.; Merdji, H.; Guizard, S.; Geoffroy, G.; Gaudin, J.; Fedorov, N.; Martin, P.; Vasil'ev, A.; Belsky, A.
2009-06-15
Exciton-exciton interaction is experimentally revealed and quantitatively analyzed in a wide band-gap scintillator material CdWO{sub 4}. Under high-intensity femtosecond vacuum ultraviolet excitation, the CdWO{sub 4} luminescence is quenched, while its decay becomes essentially nonexponential. We propose an analytical model, which successfully reproduces the decay kinetics recorded in a wide range of excitation densities. The dipole-dipole interaction between excitons leading to their nonradiative decay is shown to be the main cause of a nonproportional response common for many scintillators.
Ghost Fano Resonance of Excitons in Twisted Bilayer Graphene
NASA Astrophysics Data System (ADS)
Liang, Yufeng
2014-03-01
Metallic systems are generally considered to be unable to harbor tightly bound excitons because of the strong screening effect as well as the absence of a finite band gap. Previously, exception has only been found in one-dimensional metallic carbon nanotubes due to the depressed screening effects and the symmetry gap. We explore the exciton spectra of twisted bilayer graphene (tBLG) and predict the existence of even more strongly bound exciton (with binding energy as large as 0.5eV) in this system despite of its higher dimensionality. Based on our results from first-principles simulations and effective model calculations, a mechanism known as the ghost Fano resonance is proposed for the bound exciton formation in metallic systems beyond the dimensonality-related argument. Our results shed light on engineering the e-h excitations in the few-layer van der Waals heterojunction. NSF Grant No. DMR-1207141.
Enhanced multiple exciton generation in quasi-one-dimensional semiconductors.
Cunningham, Paul D; Boercker, Janice E; Foos, Edward E; Lumb, Matthew P; Smith, Anthony R; Tischler, Joseph G; Melinger, Joseph S
2011-08-10
The creation of a single electron-hole pair (i.e., exciton) per incident photon is a fundamental limitation for current optoelectronic devices including photodetectors and photovoltaic cells. The prospect of multiple exciton generation per incident photon is of great interest to fundamental science and the improvement of solar cell technology. Multiple exciton generation is known to occur in semiconductor nanostructures with increased efficiency and reduced threshold energy compared to their bulk counterparts. Here we report a significant enhancement of multiple exciton generation in PbSe quasi-one-dimensional semiconductors (nanorods) over zero-dimensional nanostructures (nanocrystals), characterized by a 2-fold increase in efficiency and reduction of the threshold energy to (2.23 ± 0.03)E(g), which approaches the theoretical limit of 2E(g). Photovoltaic cells based on PbSe nanorods are capable of improved power conversion efficiencies, in particular when operated in conjunction with solar concentrators.
Electrical Activation of Dark Excitonic States in Carbon Nanotubes
NASA Astrophysics Data System (ADS)
Uda, Takushi; Yoshida, Masahiro; Ishii, Akihiro; Kato, Yuichiro K.
Electrical activation of optical transitions to parity-forbidden dark excitonic states in individual carbon nanotubes is reported. We examine electric field effects on various excitonic states by simultaneously measuring both photocurrent and photoluminescence. As the applied field increases, we observe an emergence of new absorption peaks in the excitation spectra. From the diameter dependence of the energy separation between the new peaks and the ground state of E11 excitons, we attribute the peaks to the dark excited states which became optically active due to the applied field. A simple field-induced exciton dissociation model is introduced to explain the photocurrent threshold fields, and the edge of the E11 continuum states have been identified using this model. Work supported by JSPS (KAKENHI 24340066, 26610080), MEXT (Photon Frontier Network Program, Nanotechnology Platform), Canon Foundation, and Asahi Glass Foundation.
Large excitonic effects in group-IV sulfide monolayers
NASA Astrophysics Data System (ADS)
Tuttle, Blair R.; Alhassan, Saeed M.; Pantelides, Sokrates T.
2015-12-01
Large exciton binding energies are a distinguishing feature of two-dimensional semiconductors because of reduced screening, potentially leading to unique optoelectronic applications. Here we use electronic structure methods to calculate the properties of a two-dimensional material class: group-IV monosulfides including SiS, GeS, and SnS. Bulk SiS is predicted to be a metastable layered material. Quasiparticle excitations are calculated with the G0W0 method and the Bethe-Salpeter equation is are used to include electron-hole interactions. For monolayers, strongly bound excitons are found below the quasiparticle absorption edge. The predicted excitonic binding energies are as high as 0.7 eV. Due to large excitonic effects, these group-IV sulfide monolayers have great potential for nanoscale optoelectronic applications.
Singlet exciton fission-sensitized infrared quantum dot solar cells.
Ehrler, Bruno; Wilson, Mark W B; Rao, Akshay; Friend, Richard H; Greenham, Neil C
2012-02-08
We demonstrate an organic/inorganic hybrid photovoltaic device architecture that uses singlet exciton fission to permit the collection of two electrons per absorbed high-energy photon while simultaneously harvesting low-energy photons. In this solar cell, infrared photons are absorbed using lead sulfide (PbS) nanocrystals. Visible photons are absorbed in pentacene to create singlet excitons, which undergo rapid exciton fission to produce pairs of triplets. Crucially, we identify that these triplet excitons can be ionized at an organic/inorganic heterointerface. We report internal quantum efficiencies exceeding 50% and power conversion efficiencies approaching 1%. These findings suggest an alternative route to circumvent the Shockley-Queisser limit on the power conversion efficiency of single-junction solar cells.
Excitonic condensation in systems of strongly correlated electrons
NASA Astrophysics Data System (ADS)
Kuneš, Jan
2015-08-01
The idea of exciton condensation in solids was introduced in the 1960s with the analogy of superconductivity in mind. While exciton supercurrents have been realised only in artificial quantum-well structures so far, the application of the concept of excitonic condensation to bulk solids leads to a rich spectrum of thermodynamic phases with diverse physical properties. In this review we discuss recent developments in the theory of exciton condensation in systems described by Hubbard-type models. In particular, we focus on the connections to their various strong-coupling limits that have been studied in other contexts, e.g. cold atoms physics. One of our goals is to provide a ‘dictionary’ that would allow the reader to efficiently combine results obtained in these different fields.
Simulations of singlet exciton diffusion in organic semiconductors: a review
Bjorgaard, Josiah A.; Kose, Muhammet Erkan
2014-12-22
Our review describes the various aspects of simulation strategies for exciton diffusion in condensed phase thin films of organic semiconductors. Several methods for calculating energy transfer rate constants are discussed along with procedures for how to account for energetic disorder. Exciton diffusion can be modelled by using kinetic Monte-Carlo methods or master equations. Recent literature on simulation efforts for estimating exciton diffusion lengths of various conjugated polymers and small molecules are introduced. Moreover, these studies are discussed in the context of the effects of morphology on exciton diffusion and the necessity of accurate treatment of disorder for comparison of simulationmore » results with those of experiment.« less
Exciton-stimulated modulation of recombination in solar cells
Karazhanov, S.Z.
1997-12-01
This work reports an investigation of the effect of excitons on carrier recombination and solar energy conversion processes. The probabilities of exciton-stimulated modulation of the occupancy of r centers in CdS as well as the binding coefficient of free electrons and holes into excitons are estimated. Carrier recombination and transport theories are presented. The theories are applied to Cu{sub 2}S/CdS solar cells for AM1 illumination at a temperature of 300 K. It has been shown by numerical estimation that exciton-stimulated modulation of the occupancy of deep impurities does give a significant reduction of carrier recombination losses and efficiency improvements for Cu{sub 2}S/CdS solar cells. {copyright} {ital 1997 American Institute of Physics.}
Effects of Lattice Vibration on the Properties of the Strong-Coupling Polaron in a Quantum Well
NASA Astrophysics Data System (ADS)
Eerdunchaol; Xiao, J. L.
2007-04-01
In this paper, the effects of lattice vibration on the properties of the polaron, which is weakly coupled with bulk longitudinal optical (LO) phonons and strongly coupled with interface optical (IO) phonons, in an infinite quantum well are studied by means of Huybrechts’ linear-combination operator and the modified Lee-Low-Pines (LLP) variational method. The expressions for the self-trapping energy of the polaron in a quantum well as a function of the well width and temperature were derived. In particular, the law governing the change of the vibration frequency of the polaron with changing well width and temperature is obtained for the first time. Numerical results of the polaron self-trapping energy and the vibration frequency for KI/AgCl/KI QW show that the vibration frequency and the self-trapping energy of the polaron decrease with increasing well width and temperature, but the contributions of the interaction between the electron and the different branches of phonons to the self-trapping energy, the vibration frequency and the change of their variation with well width and temperature differ markedly.
NASA Astrophysics Data System (ADS)
Udal'tsov, Alexander V.
2015-11-01
Polaron theory is often used for the study of electrons and holes mobility in semiconductors when longitudinal optical (LO) phonons are generated upon the charge carriers moving. The polaron theory was applied to explain long-wavelength absorptions observed nearby Soret band in the electronic spectra of assemblies of mono-protonated meso-tetraphenylporphine dimer (TPP2H+) that are interpreted as LO-phonons originated due to proton movement. The energy of hole polaron is found to be 1.50 eV at 77 K. Energy of Franck-Condon transitions of LO-phonons generated by hole polaron moving through water confined in the assemblies with distortions of O-H bonds is 0.2653 eV (2138 cm-1). A broad band around 2127 cm-1 corresponding the same energy of O-H bonds vibrations is observed in IR spectra of the assemblies consisting of water and mainly of TPP2H+ species in the solid state indicating the presence of similar distortions of the hydrogen bonds. The radius of protonic sphere of 0.202 Å, which was estimated as a polaron quasiparticle moving through the confined water at 77 K, is found in agreement with earlier evaluated one of 0.265 Å that was obtained for proton diffusion at 298 K in similar assemblies.
Akiba, K; Kanasugi, S; Yuge, T; Nagase, K; Hirayama, Y
2015-07-10
We study nuclear spin polarization in the quantum Hall regime through the optically pumped electron spin polarization in the lowest Landau level. The nuclear spin polarization is measured as a nuclear magnetic field B(N) by means of the sensitive resistive detection. We find the dependence of B(N) on the filling factor nonmonotonic. The comprehensive measurements of B(N) with the help of the circularly polarized photoluminescence measurements indicate the participation of the photoexcited complexes, i.e., the exciton and trion (charged exciton), in nuclear spin polarization. On the basis of a novel estimation method of the equilibrium electron spin polarization, we analyze the experimental data and conclude that the filling factor dependence of B(N) is understood by the effect of electron spin polarization through excitons and trions.
Theory of lattice effects on magnetic interactions in solids
NASA Astrophysics Data System (ADS)
Meskine, Hakim
This dissertation focuses on studying the effect of lattice distortions on the magnetic properties of nickelates and manganites. These two families of materials have great potential in industrial applications in the fields of magnetic (superdense hard-drives, fast memory) and charge storage (batteries). The introduction and methods sections present the main ideas of the dissertation and discuss the various techniques used. Electron-lattice coupling is first examined in chapter three for a two-site model where we estimate the magnitude of the isotope effect on the critical temperature and show that it decreases magnetic exchange. In the next part we study electronic structure and magnetism of NaNiO2 and show that inter-planar exchange is reduced by lattice coupling. In the fifth chapter we examine the magnetic polaron and discuss the effect of static lattice coupling on its binding energy, and find it to further stabilize the polaron.
Excitonic quantum interference in a quantum dot chain with rings.
Hong, Suc-Kyoung; Nam, Seog Woo; Yeon, Kyu-Hwang
2008-04-16
We demonstrate excitonic quantum interference in a closely spaced quantum dot chain with nanorings. In the resonant dipole-dipole interaction model with direct diagonalization method, we have found a peculiar feature that the excitation of specified quantum dots in the chain is completely inhibited, depending on the orientational configuration of the transition dipole moments and specified initial preparation of the excitation. In practice, these excited states facilitating quantum interference can provide a conceptual basis for quantum interference devices of excitonic hopping.
Probing the origin of excitonic states in monolayer WSe2
Huang, Jiani; Hoang, Thang B.; Mikkelsen, Maiken H.
2016-01-01
Two-dimensional transition metal dichalcogenides (TMDCs) have spurred excitement for potential applications in optoelectronic and valleytronic devices; however, the origin of the dynamics of excitons, trions, and other localized states in these low dimensional materials is not well-understood. Here, we experimentally probed the dynamics of excitonic states in monolayer WSe2 by investigating the temperature and polarization dependent photoluminescence (PL) spectra. Four pronounced PL peaks were identified below a temperature of 60 K at near-resonant excitation and assigned to exciton, trion and localized states from excitation power dependence measurements. We find that the localized states vanish above 65 K, while exciton and trion emission peaks remain up to room temperature. This can be explained by a multi-level model developed for conventional semiconductors and applied to monolayer TMDCs for the first time here. From this model, we estimated a lower bound of the exciton binding energy of 198 meV for monolayer WSe2 and explained the vanishing of the localized states. Additionally, we observed a rapid decrease in the degree of circular polarization of the PL at increasing temperatures indicating a relatively strong electron-phonon coupling and impurity-related scattering. Our results reveal further insight into the excitonic states in monolayer WSe2 which is critical for future practical applications. PMID:26940069
Exciton energy-momentum map of hexagonal boron nitride
NASA Astrophysics Data System (ADS)
Fugallo, Giorgia; Aramini, Matteo; Koskelo, Jaakko; Watanabe, Kenji; Taniguchi, Takashi; Hakala, Mikko; Huotari, Simo; Gatti, Matteo; Sottile, Francesco
2015-10-01
Understanding and controlling the way excitons propagate in solids is a key for tailoring materials with improved optoelectronic properties. A fundamental step in this direction is the determination of the exciton energy-momentum dispersion. Here, thanks to the solution of the parameter-free Bethe-Salpeter equation (BSE), we draw and explain the exciton energy-momentum map of hexagonal boron nitride (h-BN) in the first three Brillouin zones. We show that h-BN displays strong excitonic effects not only in the optical spectra at vanishing momentum q , as previously reported, but also at large q . We validate our theoretical predictions by assessing the calculated exciton map by means of an inelastic x-ray scattering (IXS) experiment. Moreover, we solve the discrepancies between previous experimental data and calculations, proving then that the BSE is highly accurate through the whole momentum range. Therefore, these results put forward the combination BSE and IXS as the tool of choice for addressing the exciton dynamics in complex materials.
Exciton Band Structure in Two-Dimensional Materials
NASA Astrophysics Data System (ADS)
Cudazzo, Pierluigi; Sponza, Lorenzo; Giorgetti, Christine; Reining, Lucia; Sottile, Francesco; Gatti, Matteo
2016-02-01
Low-dimensional materials differ from their bulk counterparts in many respects. In particular, the screening of the Coulomb interaction is strongly reduced, which can have important consequences such as the significant increase of exciton binding energies. In bulk materials the binding energy is used as an indicator in optical spectra to distinguish different kinds of excitons, but this is not possible in low-dimensional materials, where the binding energy is large and comparable in size for excitons of very different localization. Here we demonstrate that the exciton band structure, which can be accessed experimentally, instead provides a powerful way to identify the exciton character. By comparing the ab initio solution of the many-body Bethe-Salpeter equation for graphane and single-layer hexagonal boron nitride, we draw a general picture of the exciton dispersion in two-dimensional materials, highlighting the different role played by the exchange electron-hole interaction and by the electronic band structure. Our interpretation is substantiated by a prediction for phosphorene.
Exciton Band Structure in Two-Dimensional Materials.
Cudazzo, Pierluigi; Sponza, Lorenzo; Giorgetti, Christine; Reining, Lucia; Sottile, Francesco; Gatti, Matteo
2016-02-12
Low-dimensional materials differ from their bulk counterparts in many respects. In particular, the screening of the Coulomb interaction is strongly reduced, which can have important consequences such as the significant increase of exciton binding energies. In bulk materials the binding energy is used as an indicator in optical spectra to distinguish different kinds of excitons, but this is not possible in low-dimensional materials, where the binding energy is large and comparable in size for excitons of very different localization. Here we demonstrate that the exciton band structure, which can be accessed experimentally, instead provides a powerful way to identify the exciton character. By comparing the ab initio solution of the many-body Bethe-Salpeter equation for graphane and single-layer hexagonal boron nitride, we draw a general picture of the exciton dispersion in two-dimensional materials, highlighting the different role played by the exchange electron-hole interaction and by the electronic band structure. Our interpretation is substantiated by a prediction for phosphorene.
Two-dminensional exciton states in monolayer semiconducting phosphorus alotropes
NASA Astrophysics Data System (ADS)
Rocha, Alexandre R.; Villegas, Cesar E. P.
During the last decade, novel two-dimensional (2D) semiconducting materials have been synthesized and characterised. As a result, there have been several theoretical and experimental proposals to incorporate 2D materials for designing next generation electronic and optoelectronics devices. In particular, it has been demonstrated that light absorption in phosphorus-based monolayers can span the whole visible spectrum, suggesting they could be used for optolectronic applications. A key ingredient for optolectronic applications is the presence of excitons and their subsequent diffusion along a donor material. This is influenced by the character of the different excitations taking place, as well as, the exciton binding energy. Therefore, In this work we use accurate many-body corrected density functional theory by means of GW-BSE methodology to elucidate the most important optical transitions, exciton energy spectrum as well as exciton extension in different types of phosphorene materials. In addition, we solve the Schrodinger equation for different 2D screened potentials and estimate the 2D exciton energy levels and radius extension. Finally, in order to assess further studies based on these systems, we provide a simple analityc expression for estimating 2D exciton energy levels. Research funded by FAPESP-Brazil.
Acousto-exciton interaction in a gas of 2D indirect dipolar excitons in the presence of disorder
NASA Astrophysics Data System (ADS)
Kovalev, V. M.; Chaplik, A. V.
2016-03-01
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.
Hybrid em wave - polar semiconductor interaction: A polaronic study
Paliwal, Ayushi Dubey, Swati; Ghosh, S.
2015-07-31
Present paper considers incidence of a most realistic hybrid pump wave on a weakly polar semiconductor having a very small coupling constant. Possibility of optical parametric interaction has been explored in the presence of an external transverse magnetic field. The effect of doping concentrations and transverse magnetostatic field on threshold characteristics of optical parametric interaction in polar semiconductor plasma has been studied, using hydrodynamic model of semiconductors, in the far infrared regime. Numerical estimations have been carried out by using data of weakly polar III-V GaAs semiconductor and influence of control parameters on electron-LO phonon interaction has been analyzed. A particular range of physical parameters is found to be suitable for minimum threshold. The choice of nonlinear medium and favorable range of operating parameters are crucial aspects in design and fabrication of parametric amplifiers and oscillators. The hybrid mode of the pump is found to be favorable for the onset of the said process and realization of a low cost amplifier.
Wan, Yan; Guo, Zhi; Zhu, Tong; Yan, Suxia; Johnson, Justin; Huang, Libai
2015-09-14
Singlet fission presents an attractive solution to overcome the Shockley–Queisser limit by generating two triplet excitons from one singlet exciton. Although triplet excitons are long-lived, their transport occurs through a Dexter transfer, making them slower than singlet excitons, which travel by means of a Förster mechanism. A thorough understanding of the interplay between singlet fission and exciton transport is therefore necessary to assess the potential and challenges of singlet-fission utilization. We report a direct visualization of exciton transport in single tetracene crystals using transient absorption microscopy with 200 fs time resolution and 50 nm spatial precision. Moreover, these measurements reveal a new singlet-mediated transport mechanism for triplets, which leads to an enhancement in effective triplet exciton diffusion of more than one order of magnitude on picosecond to nanosecond timescales. These results establish that there are optimal energetics of singlet and triplet excitons that benefit both singlet fission and exciton diffusion.
NASA Astrophysics Data System (ADS)
Bondarev, I. V.; Popescu, A.; Younts, R. A.; Hoffman, B.; McAfee, T.; Dougherty, D. B.; Gundogdu, K.; Ade, H. W.
2016-11-01
We report the results of the combined experimental and theoretical studies of the low-lying exciton states in crystalline copper phthalocyanine. We derive the eigen energy spectrum for the two lowest intramolecular Frenkel excitons coupled to the intermolecular charge transfer exciton state and compare it with temperature dependent optical absorption spectra measured experimentally, to obtain the parameters of the Frenkel-charge-transfer exciton intermixing. The two Frenkel exciton states 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 charge transfer exciton, showing the coupling constant 0.17 eV which agrees with earlier experimental measurements. These results can be used for the proper interpretation of the physical properties of crystalline phthalocyanines.
The nonlinear optical properties of a magneto-exciton in a strained Ga0.2In0.8As/GaAs quantum dot
NASA Astrophysics Data System (ADS)
Senthil Kumar, N R..; Peter, A. John; Kyoo, Yoo Chang
2013-10-01
The magnetic field-dependent heavy hole excitonic states in a strained Ga0.2In0.8As/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 Ga0.2In0.8As/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 Ga0.2In0.8As/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.
Temperature Dependence of the Properties of the Strong-Coupling Polaron in a Slab of Polar Crystal
NASA Astrophysics Data System (ADS)
Bao, Eerdunchaolu; Xiao, J. L.
2003-03-01
In this paper, the temperature dependence of the properties of polaron, which is weakly coupled with bulk LO phonons and strongly coupled with SO phonons, in a slab of polar crystal is studied by means of a modified second LLP transformation for the first time. An expressions for the self-trapping energy and the effective mass of the polaron in a slab of polar crystal as a function of the temperature and slab thickness are derived by using a linear combination operator and two modified LLP variational method. Our numerical results of the self-trapping energy and the effective mass for KCl show that the polaron self-trapping energy and effective mass in a polar crystal are strongly related to the slab thickness and the temperature. The self-trapping energy and the effective mass will decrease with increasing slab thickness and temperature.
Signature of polaron formation in Na0.025WO3: Photoemission and X-ray diffraction investigations
NASA Astrophysics Data System (ADS)
Paul, Sanhita; Ghosh, Anirudha; Raj, Satyabrata
2013-06-01
We have carried out temperature dependent high-resolution angle-resolved photoemission spectroscopy and x-ray diffraction studies on non-stoichiometric sodium tungsten bronzes (NaxWO3 for x=0.025). Our photoemission investigation shows evidence for polaron formation at the valence band edge and the photoemission spectra collected in different modes of the electron analyzer suggest that the density of states at valence band edge gradually moves to other k-points in the Brillouin zone with increasing temperature and explain the dynamics of polaron formation in Na0.025WO3. Infact our x-ray diffraction measurements reveal a structural modification of Na0.025WO3 around 230K. The corner sharing WO6 octadedra gets sufficiently distorted at low temperature due to displacement of tugsten and oxygen atoms from their mean position. This structural modification induces polaron formation in Na0.025WO3 below 230K.
NASA Astrophysics Data System (ADS)
Bhunia, Amit; Bansal, Kanika; Henini, Mohamed; Alshammari, Marzook S.; Datta, Shouvik
2016-10-01
Mostly, optical spectroscopies are used to investigate the physics of excitons, whereas their electrical evidences are hardly explored. Here, we examined a forward bias activated differential capacitance response of GaInP/AlGaInP based multi-quantum well laser diodes to trace the presence of excitons using electrical measurements. Occurrence of "negative activation energy" after light emission is understood as thermodynamical signature of steady state excitonic population under intermediate range of carrier injections. Similar corroborative results are also observed in an InGaAs/GaAs quantum dot laser structure grown by molecular beam epitaxy. With increasing biases, the measured differential capacitance response slowly vanishes. This represents gradual Mott transition of an excitonic phase into an electron-hole plasma in a GaInP/AlGaInP laser diode. This is further substantiated by more and more exponentially looking shapes of high energy tails in electroluminescence spectra with increasing forward bias, which originates from a growing non-degenerate population of free electrons and holes. Such an experimental correlation between electrical and optical properties of excitons can be used to advance the next generation excitonic devices.
Repulsive Fermi Polarons in a Resonant Mixture of Ultracold ^{6}Li Atoms.
Scazza, F; Valtolina, G; Massignan, P; Recati, A; Amico, A; Burchianti, A; Fort, C; Inguscio, M; Zaccanti, M; Roati, G
2017-02-24
We employ radio-frequency spectroscopy to investigate a polarized spin mixture of ultracold ^{6}Li atoms close to a broad Feshbach scattering resonance. Focusing on the regime of strong repulsive interactions, we observe well-defined coherent quasiparticles even for unitarity-limited interactions. We characterize the many-body system by extracting the key properties of repulsive Fermi polarons: the energy E_{+}, the effective mass m^{*}, the residue Z, and the decay rate Γ. Above a critical interaction, E_{+} is found to exceed the Fermi energy of the bath, while m^{*} diverges and even turns negative, thereby indicating that the repulsive Fermi liquid state becomes energetically and thermodynamically unstable.
Repulsive Fermi Polarons in a Resonant Mixture of Ultracold 6Li Atoms
NASA Astrophysics Data System (ADS)
Scazza, F.; Valtolina, G.; Massignan, P.; Recati, A.; Amico, A.; Burchianti, A.; Fort, C.; Inguscio, M.; Zaccanti, M.; Roati, G.
2017-02-01
We employ radio-frequency spectroscopy to investigate a polarized spin mixture of ultracold 6Li atoms close to a broad Feshbach scattering resonance. Focusing on the regime of strong repulsive interactions, we observe well-defined coherent quasiparticles even for unitarity-limited interactions. We characterize the many-body system by extracting the key properties of repulsive Fermi polarons: the energy E+, the effective mass m*, the residue Z , and the decay rate Γ . Above a critical interaction, E+ is found to exceed the Fermi energy of the bath, while m* diverges and even turns negative, thereby indicating that the repulsive Fermi liquid state becomes energetically and thermodynamically unstable.
Analog of small Holstein polaron in hydrogen-bonded amide systems
NASA Astrophysics Data System (ADS)
Alexander, D. M.
1985-01-01
A class of amide-I (C = O stretch) related excitations and their contribution to the spectral function for infrared absorption is determined by use of the Davydov Hamiltonian. The treatment is a fully quantum, finite-temperature one. A consistent picture and a quantitative fit to the absorption data for crystalline acetanilide confirms that the model adequately explains the anomalous behavior cited by Careri et al. The localized excitation responsible for this behavior is the vibronic analog of the small Holstein polaron. The possible extension to other modes and biological relevance is examined.
Probing excitonic dark states in single-layer tungsten disulphide.
Ye, Ziliang; Cao, Ting; O'Brien, Kevin; Zhu, Hanyu; Yin, Xiaobo; Wang, Yuan; Louie, Steven G; Zhang, Xiang
2014-09-11
Transition metal dichalcogenide (TMDC) monolayers have recently emerged as an important class of two-dimensional semiconductors with potential for electronic and optoelectronic devices. Unlike semi-metallic graphene, layered TMDCs have a sizeable bandgap. More interestingly, when thinned down to a monolayer, TMDCs transform from indirect-bandgap to direct-bandgap semiconductors, exhibiting a number of intriguing optical phenomena such as valley-selective circular dichroism, doping-dependent charged excitons and strong photocurrent responses. However, the fundamental mechanism underlying such a strong light-matter interaction is still under intensive investigation. First-principles calculations have predicted a quasiparticle bandgap much larger than the measured optical gap, and an optical response dominated by excitonic effects. In particular, a recent study based on a GW plus Bethe-Salpeter equation (GW-BSE) approach, which employed many-body Green's-function methodology to address electron-electron and electron-hole interactions, theoretically predicted a diversity of strongly bound excitons. Here we report experimental evidence of a series of excitonic dark states in single-layer WS2 using two-photon excitation spectroscopy. In combination with GW-BSE theory, we prove that the excitons are of Wannier type, meaning that each exciton wavefunction extends over multiple unit cells, but with extraordinarily large binding energy (∼0.7 electronvolts), leading to a quasiparticle bandgap of 2.7 electronvolts. These strongly bound exciton states are observed to be stable even at room temperature. We reveal an exciton series that deviates substantially from hydrogen models, with a novel energy dependence on the orbital angular momentum. These excitonic energy levels are experimentally found to be robust against environmental perturbations. The discovery of excitonic dark states and exceptionally large binding energy not only sheds light on the importance of many
Controlling exciton photophysics in single-walled carbon nanotubes
NASA Astrophysics Data System (ADS)
Sarpkaya, Ibrahim
Single-walled carbon nanotubes (SWCNTs) have been studied extensively by scientists and engineers due to their unique mechanical, optical, electronic and thermal properties that make them attractive for both fundamental research and device applications. Specifically, important optical properties of SWCNTs such as formation of strongly bound excitons (electron-hole pairs), being stable at room temperature, and bandgap-tunable light emission from visible to telecom wavelengths make them a promising material for optoelectronic and nanophotonic devices. However, the photophysics of excitons in SWCNTs is not yet fully understood and is largely affected by detrimental extrinsic effects, which give rise to strongly reduced device performance. This dissertation demonstrates novel methods and techniques to better understand and to control the photophysics of excitons in SWCNTs. The first part presents novel ways to completely remove detrimental spectral diffusion and blinking in the optical emission of surfactant dispersed SWCNTs on millisecond time scales and also demonstrates 50-fold enhanced exciton emission. Furthermore, pronounced photon antibunching is observed for the first time under resonant excitation. The demonstrated single photon emission is promising for applications in quantum cryptography, while the achieved stable long term emission is important for optoelectronic devices. The second part demonstrates a new regime of intrinsic exciton photophysics in ultra-clean SWCNTs that is characterized by ultra-narrow exciton linewidth and prolonged emission times up to 18 ns. These lifetimes are two orders of magnitude better than prior measurements and in agreement with values predicted by theorists a decade ago. Moreover, I measure for the first time exciton decoherence times of individual nanotubes in the time-domain and demonstrate fourfold prolonged values up to 2 ps compared to previous ensemble studies. Finally, I demonstrate a novel method which controls
Jahn-Teller assisted polaronic hole hopping as a charge transport mechanism in CuO nanograins
NASA Astrophysics Data System (ADS)
Younas, M.; Nadeem, M.; Idrees, M.; Akhtar, M. J.
2012-04-01
Impedance spectroscopy has been employed to investigate the dielectric and electric transport phenomena in sol-gel synthesized CuO nanograins. Semiconducting features of the grains and grain boundaries have been endorsed to the thermal activation of the localized charge carriers. On cooling below 303 K, a transition from Jahn-Teller polaron hopping mechanism to the Mott's variable range hopping mechanism has been observed owing to random potential fluctuations among localized sites. Activation energies for conduction and relaxation processes at grain boundaries provide strong signatures for the involvement of Jahn-Teller adiabatic small polarons as a charge transport mechanism in CuO nanograins.
NASA Astrophysics Data System (ADS)
Zhou, Fei; Sadigh, Babak; Erhart, Paul; Åberg, Daniel
2016-08-01
The excellent light yield proportionality of europium-doped strontium iodide (SrI2:Eu) has resulted in state-of-the-art γ-ray detectors with remarkably high-energy resolution, far exceeding that of most halide compounds. In this class of materials, the formation of self-trapped hole polarons is very common. However, polaron formation is usually expected to limit carrier mobilities and has been associated with poor scintillator light-yield proportionality and resolution. Here using a recently developed first-principles method, we perform an unprecedented study of polaron transport in SrI2, both for equilibrium polarons, as well as nascent polarons immediately following a self-trapping event. We propose a rationale for the unexpected high-energy resolution of SrI2. We identify nine stable hole polaron configurations, which consist of dimerised iodine pairs with polaron-binding energies of up to 0.5 eV. They are connected by a complex potential energy landscape that comprises 66 unique nearest-neighbour migration paths. Ab initio molecular dynamics simulations reveal that a large fraction of polarons is born into configurations that migrate practically barrier free at room temperature. Consequently, carriers created during γ-irradiation can quickly diffuse away reducing the chance for non-linear recombination, the primary culprit for non-proportionality and resolution reduction. We conclude that the flat, albeit complex, landscape for polaron migration in SrI2 is a key for understanding its outstanding performance. This insight provides important guidance not only for the future development of high-performance scintillators but also of other materials, for which large polaron mobilities are crucial such as batteries and solid-state ionic conductors.
Electrons, Phonons and Excitons at Semiconductor Surfaces
NASA Astrophysics Data System (ADS)
Pollmann, Johannes; Krueger, Peter; Mazur, Albert; Rohlfing, Michael
We briefly address 'state-of-the-art' ab-initio calculations of basic properties of semiconductor surfaces such as their atomic configuration, electronic structure and surface vibrations, as well as, their optical properties and compare exemplary results with experimental data. The surface structure and the electronic ground state are described within the local density approximation (LDA) of density functional theory (DFT). The description of excited electronic states requires to take dynamical correlations in the many electron system into account, which is achieved to a considerable extent within the GW approximation (GWA) leading to the concept of the quasiparticle bandstructure. Surface phonons are treated from first principles within density functional perturbation theory (DFPT). The theory of optical surface properties and surface excitons, in particular, requires to account for the electron-hole Coulomb correlation which is done in the framework of the Bethe-Salpeter equation (BSE). These methods yield results which are in good agreement with experiment and can significantly contribute to an interpretation of experimental data from high-resolution surface microscopy and spectroscopy thus enhancing our current understanding of semiconductor surfaces.
Plasmon transmission through excitonic subwavelength gaps.
Sukharev, Maxim; Nitzan, Abraham
2016-04-14
We study the transfer of electromagnetic energy across a subwavelength gap separating two co-axial metal nanorods. In the absence of spacer in the gap separating the rods, the system exhibits strong coupling behavior between longitudinal plasmons in the two rods. The nature and magnitude of this coupling are studied by varying various geometrical parameters. As a function of frequency, the transmission is dominated by a split longitudinal plasmon peak. The two hybrid modes are the dipole-like "bonding" mode characterized by a peak intensity in the gap and a quadrupole-like "antibonding" mode whose amplitude vanishes at the gap center. When the length of one rod is varied, this mode spectrum exhibits the familiar anti-crossing behavior that depends on the coupling strength determined by the gap width. When off-resonant 2-level emitters are placed in the gap, almost no effect on the frequency dependent transmission is observed. In contrast, when the molecular system is resonant with the plasmonic line shape, the transmission is strongly modified, showing characteristics of strong exciton-plasmon coupling. Most strongly modified is the transmission near the lower frequency "bonding" plasmon mode. The presence of resonant molecules in the gap affects not only the molecule-field interaction but also the spatial distribution of the field intensity and the electromagnetic energy flux across the junction.
Plasmon transmission through excitonic subwavelength gaps
NASA Astrophysics Data System (ADS)
Sukharev, Maxim; Nitzan, Abraham
2016-04-01
We study the transfer of electromagnetic energy across a subwavelength gap separating two co-axial metal nanorods. In the absence of spacer in the gap separating the rods, the system exhibits strong coupling behavior between longitudinal plasmons in the two rods. The nature and magnitude of this coupling are studied by varying various geometrical parameters. As a function of frequency, the transmission is dominated by a split longitudinal plasmon peak. The two hybrid modes are the dipole-like "bonding" mode characterized by a peak intensity in the gap and a quadrupole-like "antibonding" mode whose amplitude vanishes at the gap center. When the length of one rod is varied, this mode spectrum exhibits the familiar anti-crossing behavior that depends on the coupling strength determined by the gap width. When off-resonant 2-level emitters are placed in the gap, almost no effect on the frequency dependent transmission is observed. In contrast, when the molecular system is resonant with the plasmonic line shape, the transmission is strongly modified, showing characteristics of strong exciton-plasmon coupling. Most strongly modified is the transmission near the lower frequency "bonding" plasmon mode. The presence of resonant molecules in the gap affects not only the molecule-field interaction but also the spatial distribution of the field intensity and the electromagnetic energy flux across the junction.
Photosynthetic light harvesting: excitons and coherence
Fassioli, Francesca; Dinshaw, Rayomond; Arpin, Paul C.; Scholes, Gregory D.
2014-01-01
Photosynthesis begins with light harvesting, where specialized pigment–protein complexes transform sunlight into electronic excitations delivered to reaction centres to initiate charge separation. There is evidence that quantum coherence between electronic excited states plays a role in energy transfer. In this review, we discuss how quantum coherence manifests in photosynthetic light harvesting and its implications. We begin by examining the concept of an exciton, an excited electronic state delocalized over several spatially separated molecules, which is the most widely available signature of quantum coherence in light harvesting. We then discuss recent results concerning the possibility that quantum coherence between electronically excited states of donors and acceptors may give rise to a quantum coherent evolution of excitations, modifying the traditional incoherent picture of energy transfer. Key to this (partially) coherent energy transfer appears to be the structure of the environment, in particular the participation of non-equilibrium vibrational modes. We discuss the open questions and controversies regarding quantum coherent energy transfer and how these can be addressed using new experimental techniques. PMID:24352671
Benchmarking Calculations of Excitonic Couplings between Bacteriochlorophylls.
Kenny, Elise P; Kassal, Ivan
2016-01-14
Excitonic couplings between (bacterio)chlorophyll molecules are necessary for simulating energy transport in photosynthetic complexes. Many techniques for calculating the couplings are in use, from the simple (but inaccurate) point-dipole approximation to fully quantum-chemical methods. We compared several approximations to determine their range of applicability, noting that the propagation of experimental uncertainties poses a fundamental limit on the achievable accuracy. In particular, the uncertainty in crystallographic coordinates yields an uncertainty of about 20% in the calculated couplings. Because quantum-chemical corrections are smaller than 20% in most biologically relevant cases, their considerable computational cost is rarely justified. We therefore recommend the electrostatic TrEsp method across the entire range of molecular separations and orientations because its cost is minimal and it generally agrees with quantum-chemical calculations to better than the geometric uncertainty. Understanding these uncertainties can guard against striving for unrealistic precision; at the same time, detailed benchmarks can allow important qualitative questions-which do not depend on the precise values of the simulation parameters-to be addressed with greater confidence about the conclusions.
Exciton dynamics in individual semimagnetic (Zn,Mn)Te/(Zn,Mg)Te nanowires
Gałkowski, K.; Papierska, J.; Sawicki, K.; Kossacki, P.; Suffczyński, J.; Wojnar, P.; Janik, E.
2015-09-07
Dynamics and mechanisms of photocreated carriers decay in individual core/shell (Zn,Mn)Te/(Zn,Mg)Te semimagnetic nanowires are studied with a high temporal resolution. Exciton lifetime determined to 44 ± 5 ps is found to increase to 78 ± 5 ps upon application of magnetic field of up to 10 T. A quantitative modeling attributes the effects observed in time-resolved and time-integrated micro-photoluminescence to the magnetic field induced quenching of exchange Auger type, non-radiative carrier recombination related to Mn{sup 2+} ions. The reported properties of the semimagnetic nanowires are promising for their implementation in high-speed devices exploiting light-induced conductivity.
Singlet fission of hot excitons in π-conjugated polymers.
Zhai, Yaxin; Sheng, Chuanxiang; Vardeny, Z Valy
2015-06-28
We used steady-state photoinduced absorption (PA), excitation dependence (EXPA(ω)) spectrum of the triplet exciton PA band, and its magneto-PA (MPA(B)) response to investigate singlet fission (SF) of hot excitons into two separated triplet excitons, in two luminescent and non-luminescent π-conjugated polymers. From the high energy step in the triplet EXPA(ω) spectrum of the luminescent polymer poly(dioctyloxy)phenylenevinylene (DOO-PPV) films, we identified a hot-exciton SF (HE-SF) process having threshold energy at E≈2E(T) (=2.8 eV, where ET is the energy of the lowest lying triplet exciton), which is about 0.8 eV above the lowest singlet exciton energy. The HE-SF process was confirmed by the triplet MPA(B) response for excitation at E>2E(T), which shows typical SF response. This process is missing in DOO-PPV solution, showing that it is predominantly interchain in nature. By contrast, the triplet EXPA(ω) spectrum in the non-luminescent polymer polydiacetylene (PDA) is flat with an onset at E=E(g) (≈2.25 eV). From this, we infer that intrachain SF that involves a triplet-triplet pair state, also known as the 'dark' 2A(g) exciton, dominates the triplet photogeneration in PDA polymer as E(g)>2E(T). The intrachain SF process was also identified from the MPA(B) response of the triplet PA band in PDA. Our work shows that the SF process in π-conjugated polymers is a much more general process than thought previously.
Optical, Electrical and Magnetic Studies of Pi-Conjugated Organic Semiconductor Systems
Vardeny, Zeev Valentine
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.
NASA Astrophysics Data System (ADS)
Dahiya, M. S.; Khasa, S.; Yadav, Arti; Agarwal, A.
2016-05-01
Lithium bismuth borate glasses containing different amounts of cobalt and iron oxides having chemical composition xFe2O3•(20-x)CoO•30Li2O•10Bi2O3•40B2O3 (x = 0, 5, 10, 15 and 20 mol% abbreviated as CFLBB1-5 respectively) prepared via melt quench technique have been investigated for their dc electrical conductivity. The amorphous nature of prepared glasses has been confirmed through X-ray diffraction measurements. The dc electrical conductivity has been analyzed by applying Mott's small polaron hopping model. Activation energies corresponding to lower and higher temperature region have been evaluated. The iron ion concentration (N), mean spacing between iron ions (R) and polaron radius (Rp) has been evaluated using the values of phonon radius (Rph) and Debye temperature (θD). The glass sample without iron (CFLBB1) shows ionic conductivity but the incorporation of iron in the glass matrix results in the appearance of electronic conductivity.
Polaron effects on the dc- and ac-tunneling characteristics of molecular Josephson junctions
NASA Astrophysics Data System (ADS)
Wu, B. H.; Cao, J. C.; Timm, C.
2012-07-01
We study the interplay of polaronic effect and superconductivity in transport through molecular Josephson junctions. The tunneling rates of electrons are dominated by vibronic replicas of the superconducting gap, which show up as prominent features in the differential conductance for the dc and ac current. For relatively large molecule-lead coupling, a features that appears when the Josephson frequency matches the vibron frequency can be identified with an over-the-gap structure observed by Marchenkov [Nat. Nanotech. 1748-338710.1038/nnano.2007.2182, 481 (2007)]. However, we are more concerned with the weak-coupling limit, where resonant tunneling through the molecular level dominates. We find that certain features involving both Andreev reflection and vibron emission show an unusual shift of the bias voltage V at their maximum with the gate voltage Vg as V˜(2/3)Vg. Moreover, due to the polaronic effect, the ac Josephson current shows a phase shift of π when the bias eV is increased by one vibronic energy quantum ℏωv. This distinctive even-odd effect is explained in terms of the different sign of the coupling to vibrons of electrons and of Andreev-reflected holes.
Anisotropic small-polaron hopping in W:BiVO{sub 4} single crystals
Rettie, Alexander J. E.; Chemelewski, William D.; Zhou, Jianshi; Lindemuth, Jeffrey; McCloy, John S.; Marshall, Luke G.; Emin, David; Mullins, C. Buddie
2015-01-12
DC electrical conductivity, Seebeck and Hall coefficients are measured between 300 and 450 K on single crystals of monoclinic bismuth vanadate that are doped n-type with 0.3% tungsten donors (W:BiVO{sub 4}). Strongly activated small-polaron hopping is implied by the activation energies of the Arrhenius conductivities (about 300 meV) greatly exceeding the energies characterizing the falls of the Seebeck coefficients' magnitudes with increasing temperature (about 50 meV). Small-polaron hopping is further evidenced by the measured Hall mobility in the ab-plane (10{sup −1 }cm{sup 2 }V{sup −1 }s{sup −1} at 300 K) being larger and much less strongly activated than the deduced drift mobility (about 5 × 10{sup −5 }cm{sup 2 }V{sup −1 }s{sup −1} at 300 K). The conductivity and n-type Seebeck coefficient is found to be anisotropic with the conductivity larger and the Seebeck coefficient's magnitude smaller and less temperature dependent for motion within the ab-plane than that in the c-direction. These anisotropies are addressed by considering highly anisotropic next-nearest-neighbor (≈5 Å) transfers in addition to the somewhat shorter (≈4 Å), nearly isotropic nearest-neighbor transfers.
Optical Conductivity of Small Polarons in Sm1-xSrxTiO3 Epitaxial Films
NASA Astrophysics Data System (ADS)
Flaherty, William; Hauser, Adam; Law, Strange; Jackson, Clayton; Raghavan, Santosh; Isaac, Brandon; Freeze, Chris; Allen, S. James; Stemmer, Susanne
2015-03-01
We present our findings in the optical conductivity in a doping-controlled metal-to-Mott-insulator transition. These samples, grown using hybrid MBE, span the transition from the Mott insulator SmTiO3 to metallic, lightly-doped SrTiO3. Zhou and Goodenough have studied a wide range of rare earth titanates and found that SmTiO3 has thermally activated transport. We measure the optical conductivity to determine the conduction mechanism. Using FTIR spectroscopy, we extract the optical conductivity in the 0.06-2.5 eV range. If conduction in Sm1-xSrxTiO3 is due to small polarons, it will have a distinct Gaussian optical conductivity feature, related to the DC transport, as described by David Emin. Alternatively, conduction could be due to variable-range hopping between defects. Furthermore, the combination of DC and optical conductivity can test the prediction of Yee and Balents that the metal-to-insulator transition is first-order with percolative phase separation between metallic and localized regions. Such a sample would have a distinct Drude tail plus polaron contributions to its conductivity. Extreme Electron Concentration Oxide Devices, Supported by ONR N00014-12-0976.
Anisotropic small-polaron hopping in W:BiVO4 single crystals
NASA Astrophysics Data System (ADS)
Rettie, Alexander J. E.; Chemelewski, William D.; Lindemuth, Jeffrey; McCloy, John S.; Marshall, Luke G.; Zhou, Jianshi; Emin, David; Mullins, C. Buddie
2015-01-01
DC electrical conductivity, Seebeck and Hall coefficients are measured between 300 and 450 K on single crystals of monoclinic bismuth vanadate that are doped n-type with 0.3% tungsten donors (W:BiVO4). Strongly activated small-polaron hopping is implied by the activation energies of the Arrhenius conductivities (about 300 meV) greatly exceeding the energies characterizing the falls of the Seebeck coefficients' magnitudes with increasing temperature (about 50 meV). Small-polaron hopping is further evidenced by the measured Hall mobility in the ab-plane (10-1 cm2 V-1 s-1 at 300 K) being larger and much less strongly activated than the deduced drift mobility (about 5 × 10-5 cm2 V-1 s-1 at 300 K). The conductivity and n-type Seebeck coefficient is found to be anisotropic with the conductivity larger and the Seebeck coefficient's magnitude smaller and less temperature dependent for motion within the ab-plane than that in the c-direction. These anisotropies are addressed by considering highly anisotropic next-nearest-neighbor (≈5 Å) transfers in addition to the somewhat shorter (≈4 Å), nearly isotropic nearest-neighbor transfers.
Polaronic transport and current blockades in epitaxial silicide nanowires and nanowire arrays.
Iancu, Violeta; Zhang, X-G; Kim, Tae-Hwan; Menard, Laurent D; Kent, P R C; Woodson, Michael E; Ramsey, J Michael; Li, An-Ping; Weitering, Hanno H
2013-08-14
Crystalline micrometer-long YSi2 nanowires with cross sections as small as 1 × 0.5 nm(2) can be grown on the Si(001) surface. Their extreme aspect ratios make electron conduction within these nanowires almost ideally one-dimensional, while their compatibility with the silicon platform suggests application as metallic interconnect in Si-based nanoelectronic devices. Here we combine bottom-up epitaxial wire synthesis in ultrahigh vacuum with top-down miniaturization of the electrical measurement probes to elucidate the electronic conduction mechanism of both individual wires and arrays of nanowires. Temperature-dependent transport through individual nanowires is indicative of thermally assisted tunneling of small polarons between atomic-scale defect centers. In-depth analysis of complex wire networks emphasize significant electronic crosstalk between the nanowires due to the long-range Coulomb fields associated with polaronic charge fluctuations. This work establishes a semiquantitative correlation between the density and distributions of atomic-scale defects and resulting current-voltage characteristics of nanoscale network devices.
Density functional theory + U modeling of polarons in organohalide lead perovskites
NASA Astrophysics Data System (ADS)
Welch, Eric; Scolfaro, Luisa; Zakhidov, Alex
2016-12-01
We investigate the possible formation of polarons in four organic perovskites (CH3NH3PbI3, CH3NH3PbBr3, CH3NH3PbCl3, and CH3NH3PbI2Cl1) using a density functional theory (DFT) calculations with local potentials and hybrid functionals. We show that DFT+U method with U = 8 eV predicts a correct band-gap and matches the forces on ions from hybrid calculations. We then use the DFT + U approach to study the effect of polarons, i.e. to search the configuration space and locate the lowest energy localized band gap state self-trapped hole (STH). STH configurations were found for three pure halides and one mixed halide system. Spin orbit coupling (SOC) was also taken into account and the results may be found in the supplementary material. This study focuses on the +U method; however, SOC corrections added to the DFT+U calculations also resulted in STH states in all four systems.
Madelung and Hubbard interactions in polaron band model of doped organic semiconductors
Png, Rui-Qi; Ang, Mervin C.Y.; Teo, Meng-How; Choo, Kim-Kian; Tang, Cindy Guanyu; Belaineh, Dagmawi; Chua, Lay-Lay; Ho, Peter K.H.
2016-01-01
The standard polaron band model of doped organic semiconductors predicts that density-of-states shift into the π–π* gap to give a partially filled polaron band that pins the Fermi level. This picture neglects both Madelung and Hubbard interactions. Here we show using ultrahigh workfunction hole-doped model triarylamine–fluorene copolymers that Hubbard interaction strongly splits the singly-occupied molecular orbital from its empty counterpart, while Madelung (Coulomb) interactions with counter-anions and other carriers markedly shift energies of the frontier orbitals. These interactions lower the singly-occupied molecular orbital band below the valence band edge and give rise to an empty low-lying counterpart band. The Fermi level, and hence workfunction, is determined by conjunction of the bottom edge of this empty band and the top edge of the valence band. Calculations are consistent with the observed Fermi-level downshift with counter-anion size and the observed dependence of workfunction on doping level in the strongly doped regime. PMID:27582355
Photochromism and polaronic photocharge localization in diluted KTa1-xNbxO3
NASA Astrophysics Data System (ADS)
Gubaev, A. I.; Kapphan, S. E.; Jastrabik, L.; Trepakov, V. A.; Syrnikov, P. P.
2006-07-01
Ultraviolet (UV)-light-induced optical absorption in the near infrared (NIR) region was observed in diluted KTa1-xNbxO3 single crystals (x =0,0.004,0.007,0.012,0.07) at low temperatures. Illumination by wideband light (3.10-4.13eV, 300-400nm) is accompanied by the appearance of a broad NIR absorption band with the position of the maxima varying in the 0.69-0.8eV (1.54-1.79μ, T =1.3K) region for different Nb concentrations. This UV-light-induced absorption is absent in nominally pure KTaO3, as well as in all Nb diluted specimens at elevated temperatures. The centers responsible for the photochromic NIR absorption bands are tied to interband optical transitions of pair Nb4+ electronic polarons. The photochromic experimental data, supplemented by luminescence studies in the visible range, evidence the strong localization of the photocharge carriers by pair Nb4+ polarons at low temperatures. It is suggested that namely the strong localization of the photocarriers plays a crucial role in photoinduced gigantic dielectric effects and possible phase transitions, which have been recognized recently in incipient ferroelectrics at low temperatures.
Doping-Induced Absorption Bands in P3HT: Polarons and Bipolarons.
Enengl, Christina; Enengl, Sandra; Pluczyk, Sandra; Havlicek, Marek; Lapkowski, Mieczyslaw; Neugebauer, Helmut; Ehrenfreund, Eitan
2016-12-05
In this work, we focus on the formation of different kinds of charge carriers such as polarons and bipolarons upon p-type doping (oxidation) of the organic semiconductor poly(3- hexylthiophene-2,5-diyl) (P3HT). We elucidate the cyclic voltammogram during oxidation of this polymer and present spectroscopic changes upon doping in the UV/Vis/near-IR range as well as in the mid-IR range. In the low-oxidation regime, two absorption bands related to sub-gap transitions appear, one in the UV/Vis range and another one in the mid-IR range. The UV/Vis absorption gradually decreases upon further doping while the mid-IR absorption shifts to lower energy. Additionally, electron paramagnetic resonance (EPR) measurements are performed, showing an increase of the EPR signal up to a certain doping level, which significantly decreases upon further doping. Furthermore, the absorption spectra in the UV/Vis range are analyzed in relation to the morphology (crystalline vs. amorphous) by using theoretical models. Finally, the calculated charge carriers from cyclic voltammogram are linked together with optical transitions as well as with the EPR signals upon p-type doping. We stress that our results indicate the formation of polarons at low doping levels and the existence of bipolarons at high doping levels. The presented spectroscopic data are an experimental evidence of the formation of bipolarons in P3HT.
Single-electron solitons in magnetic field
NASA Astrophysics Data System (ADS)
Rudenko, M.; Svintsov, D.; Filippov, S.; Vyurkov, V.
2016-12-01
Single-electron solitons (or movable polarons) can originate near a metal surface owing to interaction with image charges. Image charges (really, surface charges) appear in response to the `instant' electron density (probability density). Interaction with metal electrodes (as well as any polarization of the environment) much affects a charge qubits functioning. To verify this theory we propose a crucial experiment based on the motion of electrons in a magnetic field in presence of weak and strong polarization.
Chiral exciton in the topological insulator Bi2Se3
NASA Astrophysics Data System (ADS)
Kung, Hsiang-Hsi; Salehi, Maryam; Wang, Xueyun; Koirala, Nikesh; Brahlek, Matthew; Lee, Alexander; Cheong, Sang-Wook; Oh, Seongshik; Blumberg, Girsh
Materials with novel band structures can host ``chiral excitons'', where the exciton emission preserves the helicity of the excitation photon, as recently demonstrated in transition metal dichalcogenide monolayers. Here, we report the observation of a highly polarized photoluminescence peak, which is due to chiral exciton emission in the topological insulator Bi2Se3. Surprisingly, the energy of the emission is centered at 2.26 eV, much higher than the 0.3 eV bulk band gap of Bi2Se3. The excitation profile shows maximum polarization around 2.60 eV excitation, suggesting the chiral exciton is due to interband transition between the topological surface states and a bulk band. We demonstrate that the polarization of the exciton emission is insensitive to temperature and Bi2Se3 film thickness, providing a convenient and robust platform for optoelectronic applications. Gb, HHK and AL acknowledge support from NSF Award DMR-1104884. MS, NK, MB and SO are funded by Gordon and Betty Moore Foundation's EPiQS initiative (GBMF4418) and NSF(DMR-1308142). XYW and SWC acknowledge support from NSF Award DMREF-1233349.
Reconfigurable exciton-plasmon interconversion for nanophotonic circuits.
Lee, Hyun Seok; Luong, Dinh Hoa; Kim, Min Su; Jin, Youngjo; Kim, Hyun; Yun, Seokjoon; Lee, Young Hee
2016-11-28
The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ∼200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ∼32 μm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of∼190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits.
Reconfigurable exciton-plasmon interconversion for nanophotonic circuits
Lee, Hyun Seok; Luong, Dinh Hoa; Kim, Min Su; Jin, Youngjo; Kim, Hyun; Yun, Seokjoon; Lee, Young Hee
2016-01-01
The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ∼200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ∼32 μm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of∼190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits. PMID:27892463
Reconfigurable exciton-plasmon interconversion for nanophotonic circuits
NASA Astrophysics Data System (ADS)
Lee, Hyun Seok; Luong, Dinh Hoa; Kim, Min Su; Jin, Youngjo; Kim, Hyun; Yun, Seokjoon; Lee, Young Hee
2016-11-01
The recent challenges for improving the operation speed of nanoelectronics have motivated research on manipulating light in on-chip integrated circuits. Hybrid plasmonic waveguides with low-dimensional semiconductors, including quantum dots and quantum wells, are a promising platform for realizing sub-diffraction limited optical components. Meanwhile, two-dimensional transition metal dichalcogenides (TMDs) have received broad interest in optoelectronics owing to tightly bound excitons at room temperature, strong light-matter and exciton-plasmon interactions, available top-down wafer-scale integration, and band-gap tunability. Here, we demonstrate principal functionalities for on-chip optical communications via reconfigurable exciton-plasmon interconversions in ~200-nm-diameter Ag-nanowires overlapping onto TMD transistors. By varying device configurations for each operation purpose, three active components for optical communications are realized: field-effect exciton transistors with a channel length of ~32 μm, field-effect exciton multiplexers transmitting multiple signals through a single NW and electrical detectors of propagating plasmons with a high On/Off ratio of~190. Our results illustrate the unique merits of two-dimensional semiconductors for constructing reconfigurable device architectures in integrated nanophotonic circuits.
Multiple Exciton Generation in Semiconductor Nanostructures: DFT-based Computation
NASA Astrophysics Data System (ADS)
Mihaylov, Deyan; Kryjevski, Andrei; Kilin, Dmitri; Kilina, Svetlana; Vogel, Dayton
Multiple exciton generation (MEG) in nm-sized H-passivated Si nanowires (NWs), and quasi 2D nanofilms depends strongly on the degree of the core structural disorder as shown by the perturbation theory calculations based on the DFT simulations. In perturbation theory, we work to the 2nd order in the electron-photon coupling and in the (approximate) RPA-screened Coulomb interaction. We also include the effect of excitons for which we solve Bethe-Salpeter Equation. To describe MEG we calculate exciton-to-biexciton as well as biexciton-to-exciton rates and quantum efficiency (QE). We consider 3D arrays of Si29H36 quantum dots, NWs, and quasi 2D silicon nanofilms, all with both crystalline and amorphous core structures. Efficient MEG with QE of 1.3 up to 1.8 at the photon energy of about 3Egap is predicted in these nanoparticles except for the crystalline NW and film where QE ~=1. MEG in the amorphous nanoparticles is enhanced by the electron localization due to structural disorder. The exciton effects significantly red-shift QE vs. photon energy curves. Nm-sized a-Si NWs and films are predicted to have effective MEG within the solar spectrum range. Also, we find efficient MEG in the chiral single-wall Carbon nanotubes and in a perovskite nanostructure.
Two-dimensional exciton properties in monolayer semiconducting phosphorus allotropes.
Villegas, Cesar E P; Rodin, A S; Carvalho, Alexandra; Rocha, A R
2016-10-12
Excitons play a key role in technological applications since they have a strong influence on determining the efficiency of photovoltaic devices. Recently, it has been shown that the allotropes of phosphorus possess an optical band gap that can be tuned over a wide range of values including the near-infrared and visible spectra, which would make them promising candidates for optoelectronic applications. In this work we carry out ab initio many-body perturbation theory calculations to study the excitonic effects on the optical properties of two-dimensional phosphorus allotropes: the case of blue and black monolayers. We elucidate the most relevant optical transitions, exciton binding energy spectrum as well as real-space exciton distribution, particularly focusing on the absorption spectrum dependence on the incident light polarization. In addition, based on our results, we use a set of effective hydrogenic models, in which the electron-hole Coulomb interaction is included to estimate exciton binding energies and radii. Our results show an excellent agreement between the many-body methodology and the effective models.
Incoherent exciton trapping in self-similar aperiodic lattices
Dominguez-Adame, F.; Macia, E. ); Sanchez, A. Escuela Politecnica Superior, Universidad Carlos III de Madrid, C./Butarque 15, E-28911 Leganes, Madrid )
1995-01-01
Incoherent exciton dynamics in one-dimensional perfect lattices with traps at sites arranged according to aperiodic deterministic sequences is studied. We focus our attention on Thue-Morse and Fibonacci systems as canonical examples of self-similar aperiodic systems. Solving numerically the corresponding master equation we evaluate the survival probability and the mean-square displacement of an exciton initially created at a single site. Results are compared to systems of the same size with the same concentration of traps randomly as well as periodically distributed over the whole lattice. Excitons progressively extend over the lattice on increasing time and, in this sense, they act as a probe of the particular arrangements of traps in each system considered. The analysis of the characteristic features of their time decay indicates that exciton dynamics in self-similar aperiodic arrangements of traps is quite close to that observed in periodic ones, but differs significantly from that corresponding to random lattices. We also report on characteristic features of exciton motion suggesting that Fibonacci and Thue-Morse orderings might be clearly observed by appropriate experimental measurements. In the conclusions we comment on the implications of our work on the way towards a unified theory of the ordering of matter.
Interface exciton at lateral heterojunction of monolayer semiconductors
NASA Astrophysics Data System (ADS)
Lau, Ka Wai; Gong, Zhirui; Yu, Hongyi; Yao, Wang
Heterostructures based on 2D transition metal dichalcogenides (TMDs) have attracted extensive research interest recently due to the appealing physical properties of TMDs and new geometries for forming heterostructures. One such heterostructure is the lateral heterojunctions seamlessly formed in a monolayer crystal between two different types of TMDs, e.g. WSe2 and MoSe2. Such heterojunction exhibits a type II band alignment, with electrons (holes) having lower energy on the MoSe2 (WSe2) region. Here we present the study of an interface exciton at the 1D lateral junction of monolayer TMDs. With the distance dependent screening, we find that the interface exciton can have strong binding even though the electron-hole separation is much larger compare to the 2D excitons in TMDs. Neutral excitons are studied using two different approaches: the solution based on a real-space tight binding model, and the perturbation expansion in a hydrogen-like basis in an effective mass model. We have also used the latter method to study charged excitons at a MoSe2-WSe2-MoSe2 nanoscale junction. The work is supported by the Research Grant Council of Hong Kong (HKU705513P, HKU9/CRF/13G), the Croucher Foundation, and the HKU OYRA.
NASA Astrophysics Data System (ADS)
Zhao, Feng-qi; Guo, Zi-Zheng; Zhu, Jun
2016-10-01
The influence of the built-in electric field on the binding energy of a bound polaron and the polaron effect in a wurtzite ZnO/MgxZn1-xO quantum well are studied using the improved Lee-Low-Pines intermediate coupling method. The ground-state binding energy, the contributions from different branches of optical phonons to the energy and the binding energy are presented as the functions of well width, impurity position and composition. In the numerical calculations, the anisotropic properties of the frequencies of the different branches of optical phonons, electron effective mass, dielectric constant, the electron-optical phonon interaction and the impurity center-optical phonon interaction are considered. The results show that the built-in electric field has obvious influence on the energy, the binding energy and the polaron effect, and it affects the contributions of different phonon modes to the energy and the binding energy with different degrees. The built-in electric field significantly increases the total phonon contribution to the energy, but it reduces the total phonon contribution to the binding energy. The binding energy of the bound polaron with the built-in electric field is less than that without the built-in electric field, and it declines rapidly with increasing well width. Because of the built-in electric field effects, the contributions from different branches of phonons to the energy and the binding energy and the functions of binding energy with well width and impurity center position are different from the cases without the built-in electric field. The built-in electric field in the wurtzite ZnO/MgxZn1-xO quantum wells has a great impact on the binding energy and polaron effect, and the polaron effect in the wurtzite ZnO/MgxZn1-xO quantum wells is significantly greater than that in the zinc blende GaAs/AlxGa1-xAs QWs, hence, it is necessary to discuss the built-in electric field and polaron effect when considering the problem of electronic state
Novel Quantum Condensates in Excitonic Matter
NASA Astrophysics Data System (ADS)
Littlewood, P. B.; Keeling, J. M. J.; Simons, B. D.; Eastham, P. R.; Marchetti, F. M.; Szymańska, M. H.
2009-08-01
These lectures interleave discussion of a novel physical problem of a new kind of condensate with teaching of the fundamental theoretical tools of quantum condensed matter field theory. Polaritons and excitons are light mass composite bosons that can be made inside solids in a number of different ways. As bosonic particles, they are liable to make a phase coherent ground state—generically called a Bose-Einstein condensate (BEC)—and these lectures present some models to describe that problem, as well as general approaches to the theory. The focus is very much to explain how mean-field-like approximations that are often presented heuristically can be derived in a systematic fashion by path integral methods. Going beyond the mean field theory then produces a systematic approach to calculation of the excitation energies, and the derivation of effective low energy theories that can be generalised to more complex dynamical and spatial situations than is practicable for the full theory, as well as to study statistical properties beyond the semi-classical regime. in particular, for the polariton problem, it allows one to connect the regimes of equilibrium BEC and non-equilibrium laser. The lectures are self-sufficient, but not highly detailed. The methodological aspects are covered in standard quantum field theory texts and the presentation here is deliberately cursory: the approach will be closest to the book of Altland and Simons [1]. Since these lectures concern a particular type of condensate, reference should also be made to texts on BEC, for example by Pitaevskii and Stringari [2]. A recent theoretically focussed review of polariton systems is [3] covers many of the technical issues associated with the polariton problem in greater depth and provides many further references.
Yu, Hongyi; Liu, Gui-Bin; Gong, Pu; Xu, Xiaodong; Yao, Wang
2014-05-12
In monolayer transition metal dichalcogenides, tightly bound excitons have been discovered with a valley pseudospin optically addressable through polarization selection rules. Here, we show that this valley pseudospin is strongly coupled to the exciton centre-of-mass motion through electron-hole exchange. This coupling realizes a massless Dirac cone with chirality index I = 2 for excitons inside the light cone, that is, bright excitons. Under moderate strain, the I = 2 Dirac cone splits into two degenerate I = 1 Dirac cones, and saddle points with a linear Dirac spectrum emerge. After binding an extra electron, the charged exciton becomes a massive Dirac particle associated with a large valley Hall effect protected from intervalley scattering. Our results point to unique opportunities to study Dirac physics, with exciton's optical addressability at specifiable momentum, energy and pseudospin. The strain-tunable valley-orbit coupling also implies new structures of exciton condensates, new functionalities of excitonic circuits and mechanical control of valley pseudospin.
Rörich, Irina; Mikhnenko, Oleksandr V; Gehrig, Dominik; Blom, Paul W M; Crăciun, N Irina
2017-02-16
Using time-resolved photoluminescence (TRPL) spectroscopy the exciton lifetime in a range of conjugated polymers is investigated. For poly(p-phenylenevinylene) (PPV)-based derivatives and a polyspirobifluorene copolymer (PSBF) we find that the exciton lifetime is correlated with the energetic disorder. Better ordered polymers exhibit a single exponential PL decay with exciton lifetimes of a few hundred picoseconds, whereas polymers with a larger degree of disorder show multiexponential PL decays with exciton lifetimes in the nanosecond regime. These observations are consistent with diffusion-limited exciton quenching at nonradiative recombination centers. The measured PL decay time reflects the time that excitons need to diffuse toward these quenching sites. Conjugated polymers with large energetic disorder and thus longer exciton lifetime also exhibit a higher photoluminescence quantum yield due to the slower exciton diffusion toward nonradiative quenching sites.
NASA Astrophysics Data System (ADS)
Hu, Hui; Wang, An-Bang; Yi, Su; Liu, Xia-Ji
2016-05-01
We theoretically investigate the behavior of a moving impurity immersed in a sea of fermionic atoms that are confined in a quasiperiodic (bichromatic) optical lattice within a standard variational approach. We consider both repulsive and attractive contact interactions for such a simple many-body localization problem of Fermi polarons. The variational approach enables us to access relatively large systems and therefore may be used to understand many-body localization in the thermodynamic limit. The energy and wave function of the polaron states are found to be strongly affected by the quasirandom lattice potential and their experimental measurements (i.e., via radio-frequency spectroscopy or quantum gas microscope) therefore provide a sensitive way to underpin the localization transition. We determine a phase diagram by calculating two critical quasirandom disorder strengths, which correspond to the onset of the localization of the ground-state polaron state and the many-body localization of all polaron states, respectively. Our predicted phase diagram could be straightforwardly examined in current cold-atom experiments.
Kinetics of light-induced polaron- and VIS-centers in SBN:Ce single crystals at low temperature
NASA Astrophysics Data System (ADS)
Gubaev, A.; Kapphan, S.; Kislova, I.; Kutsenko, A.; Pankrath, R.; Vikhnin, V.
2005-01-01
The promising photorefractive crystal SrxBa1-xNb2O6 (SBN, congruent composition x = 0.61) can be doped with polyvalent ions like Ce to enhance photorefractive properties. Illumination with blue Ar+-laser light at low temperature creates light-induced NIR and VIS absorption bands. The NIR absorption has been identified as being due to Nb4+ electron polarons and their properties have been investigated in some detail. The VIS-Centers are less well understood and their nature is still under discussion. It has been shown by our previous measurements that illumination with red Kr+-laser light (647 nm) or red laser diodes (673 nm) leads to a dissociation of the VIS-Centers and a simultaneous build-up of a transient NIR-polaron absorption. We report here some new facts important for the simplified charge transfer model needed to describe quantitatively the equilibrium values and the dynamics of the NIR-polaron and VIS-center absorption. These features give new insight into the dynamic nature of these VIS-centers, which are currently being discussed as either bipolarons (in analogy to LiNbO3) or polarons trapped at charged centers, or charge transfer vibronic exitons (CTVEs) being trapped at charged centers.
Charged two-exciton emission from a single semiconductor nanocrystal
Hu, Fengrui; Zhang, Qiang; Zhang, Chunfeng; Wang, Xiaoyong; Xiao, Min
2015-03-30
Here, we study the photoluminescence (PL) time trajectories of single CdSe/ZnS nanocrystals (NCs) as a function of the laser excitation power. At the low laser power, the PL intensity of a single NC switches between the “on” and “off” levels arising from the neutral and positively charged single excitons, respectively. With the increasing laser power, an intermediate “grey” level is formed due to the optical emission from a charged multiexciton state composed of two excitons and an extra electron. Both the inter-photon correlation and the PL decay measurements demonstrate that lifetime-indistinguishable photon pairs are emitted from this negatively charged two-exciton state.
Indirect excitons in hydrogen-doped ZnO
NASA Astrophysics Data System (ADS)
Zhu, Liangchen; Lem, Laurent L. C.; Nguyen, Thien-Phap; Fair, Kit; Ali, Sajid; Ford, Michael J.; Phillips, Matthew R.; Ton-That, Cuong
2017-03-01
We present a correlative experimental and theoretical study of bound excitons in hydrogen-doped ZnO, with a particular focus on the dynamics of their metastable state confined in the sub-surface region, using a combination of surface-sensitive characterisation techniques and density functional theory calculations. A metastable sub-surface emission at 3.31 eV found in H-doped ZnO is attributed to the radiative recombination of indirect excitons localised at basal plane stacking faults (BSFs) where the excitonic transition involves electrons bound to bond-centre hydrogen donors in the potential well of the BSF. Additionally, our work shows the electrical transport of ZnO Schottky junctions is dominated by electrons confined at BSFs in the near-surface region.
Quantum confinement-induced tunable exciton states in graphene oxide
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. PMID:23872608
Huge excitonic effects in layered hexagonal boron nitride.
Arnaud, B; Lebègue, S; Rabiller, P; Alouani, M
2006-01-20
The all-electron GW approximation energy band gap of bulk hexagonal boron nitride is shown to be of indirect type. The resulting computed in-plane polarized optical spectrum, obtained by solving the Bethe-Salpeter equation for the electron-hole two-particle Green function, is in excellent agreement with experiment and has a strong anisotropy compared to out-of-plane polarized spectrum. A detailed analysis of the excitonic structures within the band gap shows that the low-lying excitons belong to the Frenkel class and are tightly confined within the layers. The calculated exciton binding energy is much larger than that obtained by Watanabe et al. [Nat. Mater. 3, 404 (2004).] based on a Wannier model assuming h-BN to be a direct-band-gap semiconductor.
Exciton coupling induces vibronic hyperchromism in light-harvesting complexes
NASA Astrophysics Data System (ADS)
Schulze, Jan; Torbjörnsson, Magne; Kühn, Oliver; Pullerits, Tõnu
2014-04-01
The recently suggested possibility that weak vibronic transitions can be excitonically enhanced in light-harvesting complexes is studied in detail. A vibronic exciton dimer model that includes ground-state vibrations is investigated using the multi-configuration time-dependent Hartree method with a parameter set typical to photosynthetic light-harvesting complexes. The absorption spectra are discussed based on the Coulomb coupling, the detuning of the site energies, and the number of vibrational modes. Fluorescence spectra calculations show that the spectral densities obtained from the low-temperature fluorescence line-narrowing measurements of light-harvesting systems need to be corrected for the effects of excitons. For the J-aggregate configuration, as in most light-harvesting complexes, the true spectral density has a larger amplitude than that obtained from the measurement.