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Sample records for excitonic magnetic polarons

  1. Excitonic polarons in low-dimensional transition metal dichalcogenides

    NASA Astrophysics Data System (ADS)

    Thilagam, A.

    2015-05-01

    We examine the excitonic polaron properties of common monolayer transition metal dichalcogenides (MoS2, MoSe2, WS2 and WSe2). The excitonic polaron is formed when excitons interact with acoustic or optical phonons via coupling to the deformation potentials associated with the conduction and valence bands. A unitary transformation which performs an approximate diagonalization of the exciton-phonon operator is used to evaluate the ground state energy of the excitonic polaron. We derive analytical expressions of the changes in the excitonic polaron energy and mass at small exciton wavevectors involving the deformation potential due to optical phonons. The polaronic effect of the monolayer transition metal dichalcogenides is examined by comparing changes in the energy gap shift and effective masses based on known deformation potential constants for carrier-phonon interactions. Our results indicate the occurrence of comparable energy shifts when the ground state exciton interacts with optical or acoustic phonons. We extend our calculations to explore the influence of exciton-lattice interactions on the binding energies and the self-trapping of excitons in two-dimensional layers of transition metal dichalcogenides.

  2. Time-resolved photoluminescence spectroscopy of localized exciton magnetic polarons in Cd{sub 0.70}Mn{sub 0.30}Te spin glass compound

    SciTech Connect

    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.

  3. Dynamics of Photogenerated Polaron-Excitons in Organic Semiconductors

    NASA Astrophysics Data System (ADS)

    Junior, Luiz A. Ribeiro; Neto, Pedro H. Oliveira; da Cunha, Wiliam F.; Silva, Geraldo M. e.

    In this work we performed numerical simulations of one π-conjugated polymer chain subjected to photogeneration. Within the SSH model modified to include the Brazoviskii-Kirova symmetry breaking term, we investigate the dynamics of photoexcitations to address the generation mechanism of polaron-excitons using the unrestricted Hartree-Fock approximation. It was obtained that after the photoexcitation the system relaxes spontaneously into a polaron-exciton in a transient state in a range of 200 fs. Our results also show that charged polarons are generated directly after this transient state.

  4. Transient spectroscopy of excitons and polarons in C[sub 60] films from femtoseconds to milliseconds

    SciTech Connect

    Dick, D.; Wei, X.; Jeglinski, S.; Benner, R.E.; Vardeny, Z.V. ); Moses, D.; Srdanov, V.I.; Wudl, F. )

    1994-11-14

    We have studied photoexcitations in C[sub 60] films using transient photomodulation and photoluminescence from 100 fs to 50 ms and absorption-detected magnetic resonance (ADMR). We show that singlet Frenkel excitons are the primary photoexcitations; their recombination kinetics in the picosecond time domain are dispersive as a result of inhomogeneity. The long-lived photoexcitations, however, are shown to be triplet excitons and charged polarons (C[sub 60][sup [minus plus

  5. Excitons, polarons, and laser action in poly(p-phenylene vinylene) films

    NASA Astrophysics Data System (ADS)

    Österbacka, R.; Wohlgenannt, M.; Shkunov, M.; Chinn, D.; Vardeny, Z. V.

    2003-05-01

    We have used a multitude of linear and nonlinear cw optical spectroscopies to study the optical properties of water precursor poly(p-phenylene vinylene) (PPV) thin films. These spectroscopies include absorption, photoluminescence, photoinduced absorption and their respective optically detected magnetic resonance, and electroabsorption spectroscopy. We have studied singlet and triplet excitons, polarons, and laser action in PPV films. We found that the lowest-lying absorption band is excitonic in origin. It consists of two absorption components due to a bimodal distribution of the polymer chain conjugation lengths. Electroabsorption spectroscopy unambiguously shows the positions of the lowest-lying odd parity exciton 1Bu at 2.59 eV and two of the higher-lying even-parity excitons, namely, mAg at 3.4 eV and kAg at 3.7 eV. From these exciton energies we obtained a lower bound for the exciton binding energy in PPV, Eb(min)=E(mAg)-E(1Bu)=0.8 eV. The quantum efficiency spectrum for triplet exciton photogeneration consists of two contributions; the intersystem crossing and, at higher energies, singlet fission. From the onset of the singlet fission process at ESF=2ET, we could estimate the energy of the lowest-lying triplet exciton, 1 3Bu, at 1.55 eV, with a singlet-triplet splitting as large as 0.9 eV. From photoinduced absorption spectroscopy we measured the triplet-triplet transition, T→T*, to be 1.45 eV. The quantum efficiency spectrum for polaron photogeneration also consists of two contributions: one extrinsic and the other intrinsic. The latter shows a monotonically increasing function of energy with an energy onset at 3.3 eV. The intrinsic photogeneration process is analyzed with a model of free-electron-hole pair photogeneration, which separate more effectively at higher energy. The carrier generation quantum yield at 3.65 eV is estimated to be 0.5%. The quantum efficiency for photoluminescence, on the other hand, shows one single step-function process, with an

  6. Reducing exciton-polaron annihilation in organic planar heterojunction solar cells

    NASA Astrophysics Data System (ADS)

    Verreet, Bregt; Bhoolokam, Ajay; Brigeman, Alyssa; Dhanker, Rijul; Cheyns, David; Heremans, Paul; Stesmans, Andre; Giebink, Noel C.; Rand, Barry P.

    2014-09-01

    We investigate the relationship between charge concentration, exciton concentration, and photocurrent generation in fullerene-containing heterojunction diodes. Impedance measurements on C60 diodes reveal a charge buildup at the C60/bathocuproine (BCP) interface that can be swept out under reverse bias. In solar cell structures, a similar charge buildup is observed in dark conditions, and increases as a function of incident light intensity. Photoluminescence measurements reveal that the C60 exciton concentration is voltage dependent, explained via the process of exciton-polaron annihilation. This process has a negative impact on the generated photocurrent of the solar cells and thereby decreases the fill factor. A combination of electroabsorption, photoluminescence, and impedance measurements reveal a decrease in charge buildup and the associated exciton-polaron annihilation through the use of a BCP/3,4,9,10-perylenetetracarboxylic bis-benzimidazole/Ag cathode.

  7. Negative Polaron and Triplet Exciton Diffusion inOrganometallic “Molecular Wires”

    SciTech Connect

    Schanze, K.S.; Miller, J.; Keller, J.M.; Sean McIlroy, S.; Sreearuothai, P.; Danilov, E.O.; Jiang, H.; Glusac, K.D.; Miller, J.R.

    2011-07-27

    The dynamics of negative polaron and triplet exciton transport within a series of monodisperse platinum (Pt) acetylide oligomers is reported. The oligomers consist of Pt-acetylide repeats, [PtL{sub 2}-C {triple_bond} C-Ph-C {triple_bond} C-]{sub n} (where L = PBu{sub 3} and Ph = 1,4-phenylene, n = 2, 3, 6, and 10), capped with naphthalene diimide (NDI) end groups. The Pt-acetylide segments are electro- and photoactive, and they serve as conduits for transport of electrons (negative polaron) and triplet excitons. The NDI end groups are relatively strong acceptors, serving as traps for the carriers. Negative polaron transport is studied by using pulse radiolysis/transient absorption at the Brookhaven National Laboratory Laser-Electron Accelerator Facility (LEAF). Electrons are rapidly attached to the oligomers, with some fraction initially residing upon the Pt-acetylide chains. The dynamics of transport are resolved by monitoring the spectral changes associated with transfer of electrons from the chain to the NDI end group. Triplet exciton transport is studied by femtosecond-picosecond transient absorption spectroscopy. Near-UV excitation leads to rapid production of triplet excitons localized on the Pt-acetylide chains. The excitons transport to the chain ends, where they are annihilated by charge separation with the NDI end group. The dynamics of triplet transport are resolved by transient absorption spectroscopy, taking advantage of the changes in spectra associated with decay of the triplet exciton and rise of the charge-separated state. The results indicate that negative polarons and excitons are transported rapidly, on average moving distances of 3 nm in less than 200 ps. Analysis of the dynamics suggests diffusive transport by a site-to-site hopping mechanism with hopping times of 27 ps for triplets and <10 ps for electrons.

  8. Reentrant formation of magnetic polarons in quantum dots

    NASA Astrophysics Data System (ADS)

    Pientka, J. M.; Oszwałdowski, R.; Petukhov, A. G.; Han, J. E.; Žutić, Igor

    2012-10-01

    We propose a model of magnetic polaron formation in semiconductor quantum dots doped with magnetic ions. A wetting layer serves as a reservoir of photogenerated holes, which can be trapped by the adjacent quantum dots. For certain hole densities, the temperature dependence of the magnetization induced by the trapped holes is reentrant: it disappears for some temperature range and reappears at higher temperatures. We demonstrate that this peculiar effect is not an artifact of the mean-field approximation and persists after statistical spin fluctuations are accounted for. We predict fingerprints of reentrant magnetic polarons in photoluminescence spectra.

  9. Magnetization steps and bound magnetic polarons in diluted magnetic semiconductors

    NASA Astrophysics Data System (ADS)

    McCabe, Gao Hua

    1997-09-01

    Magnetization measurements and computer simulations were used to address several current problems in the area of the Diluted Magnetic Semiconductors (DMS). The method of Magnetization Steps (MSTs) was used to study Jahn-Teller Distortions in Zn1-xCrxTe, and exchange constants in Pb1-xEuxSe and Pb1- xEuxTe. Bound magnetic polarons in Cu2MnxZn1-xSnS4 were studied by conventional magnetometry. Jahn-Teller Distortions in cubic Zn1- xCrxTe were studied using MSTs. Possible Jahn- Teller Distortions in this material are along the three equivalent /langle 100/rangle axes. Energy states for the three distortion directions are equivalent at H = 0, but are different for finite H. The main issue is whether the populations of three possible distortions will vary with field, or remain frozen at their values in zero- field. The data showed that the populations of the distortions changed significantly. The dominant antiferomagnetic exchange constants J between Eu2+ ions in IV-VI Pb1- xEuxSe and Pb1-xEuxTe were determined using the MST method. Measurements were made at 0.6 K in fields up to 150 kOe. Supplementary data by our collaborators were taken at much lower temperatures. Simulations of various MSTs (from isolated Eu2+ ions, pairs of ions, and triplets) were performed to fit the experimental data. Because J is determined from the MSTs for pairs, the effects of other anisotropies and exchange interactions on these MSTs were considered. They were found to bring little change to the values of J. The exchange constants were J/kB = -0/24 ± 0.03 K for Ph 1-xEu xSe amd os J/KB = -0.264 ± 0.018 K for Ph1-xEuxTe. The dominant AF exchange constants were identified as J1, between nearest-neighbors, by comparing the experimental magnetization curves to the theoretical simulations using the single J model. The dominant antiferromagnetic exchange constants J between Eu2+ ions in IV-VI Pb1- xEuxSe and Pb1-xEuxTe were determined using the MST method. Measurements were made at 0.6 K in

  10. Magnetic frustration in itinerant systems: the Kondo polaron problem

    NASA Astrophysics Data System (ADS)

    Isaev, Leonid; Batista, Cristian; Vekhter, Ilya

    2013-03-01

    We study the interplay between magnetic frustration and Kondo screening in Kondo lattices by analyzing the J1-J2 antiferromagnetic chain coupled to a conduction band. The system is tuned to the Majumdar-Ghosh point J2 =J1 / 2 which stabilizes a dimer valence-bond solid at weak Kondo coupling JK. We use an effective low-energy theory to demonstrate that sufficiently large JK results in a proliferation of ``Kondo polarons'', i.e. Kondo-screened domain-wall excitations of the dimer state, and collapse of the dimer order via a 2nd order quantum phase transition. At the quantum critical point, JK =JKc , these polarons become gapless, and we argue that the transition itself belongs to a 2D Ising universality class. For JK >JKc increasing concentration of the polarons leads to a continuous growth of the electron Fermi momentum until all spins are absorbed by the Fermi sea.

  11. Singlet and triplet excitons and charge polarons in cycloparaphenylenes: a density functional theory study.

    PubMed

    Liu, Jin; Adamska, Lyudmyla; Doorn, Stephen K; Tretiak, Sergei

    2015-06-14

    The 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. PMID:25971627

  12. Singlet and triplet excitons and charge polarons in cycloparaphenylenes. A density functional theory study

    DOE PAGES

    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.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

  13. Singlet and triplet excitons and charge polarons in cycloparaphenylenes. A density functional theory study

    SciTech Connect

    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.

  14. Long-lived localized magnetic polarons in ZnMnSe/ZnSSe type-II superlattices

    SciTech Connect

    Maksimov, A. A. Pashkov, A. V.; Brichkin, A. S.; Kulakovskii, V. D.; Tartakovskii, I. I.; Toropov, A. A.; Ivanov, S. V.

    2008-06-15

    The kinetics and polarized spectra of low-temperature photoluminescence in semiconductor type-II superlattices based on ZnMnSe/ZnSSe structures have been studied in detail. Processes responsible for the formation of short-lived (about 1 ns) and long-lived (above 10 ns) localized exciton-type magnetic polarons (EMPs) in these systems are determined, and the relative contributions due to magnetic and nonmagnetic localization of heavy holes to the formation of such polarons are evaluated. A phenomenological model is constructed that takes into account the energy distribution of charge-carrier traps with respect to their level depths and employs the EMP parameters determined for ZnMnSe quantum wells. Within the proposed model, all spectral, temporal, and temperature-dependent features in the behavior of magnetophotoluminescence observed for the system under consideration can be consistently and quantitatively described.

  15. The origin of ferromagnetic interaction between bound magnetic polarons in diluted magnetic semiconductors: A minimal model

    NASA Astrophysics Data System (ADS)

    Bednarski, Henryk

    2014-01-01

    We present a detailed analysis of the role of various interaction mechanisms contributing to the bound magnetic polaron (BMP) molecule Hamiltonian with the purpose of gaining an insight into the origin of the ferromagnetic interaction between BMPs. Explicitly, it appears that the BMP molecule Hamiltonian without interatomic direct exchange interaction does not lead to appearance of the parallel alignment of polaronic clouds in the lowest energy state even for large magnitudes of the polaronic exchange fields (up to ~65 meV in Cd0.95Mn0.05Se). Also, it appears that for the range of moderate values of polaronic exchange fields (16-25 meV in Cd0.95Mn0.05Se), the regular Hubbard BMP pair Hamiltonian must be supplemented with the direct interatomic (Heisenberg) exchange interaction to form a minimal model Hamiltonian of BMP molecule with the parallel alignment of the polaronic clouds in the lowest energy state.

  16. Magnetic monopole polarons in artificial spin ices

    NASA Astrophysics Data System (ADS)

    Chern, Gia-Wei; Mellado, Paula

    2016-05-01

    Emergent quasiparticles that arise from the fractionalization of the microscopic degrees of freedom have been one of the central themes in modern condensed-matter physics. The notion of magnetic monopoles, freely moving quasiparticles fragmented from local dipole excitations, has enjoyed much success in understanding the thermodynamic, static, and transport properties of the so-called spin-ice materials. The artificial version of spin ice, where a lattice of nanoscale magnetic dipoles is sculpted out of a ferromagnetic film, provides a unique opportunity to study these unusual quasiparticles in a material-by-design approach. Here we show that the elementary excitations in the ice phase of a nano-magnetic array arranged in the pentagonal lattice are composite objects comprised of the emergent monopole and a surrounding cloud of opposite uncompensated magnetic charges.

  17. Magnetic-Polaron-Induced Enhancement of Surface Raman Scattering

    PubMed Central

    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

  18. Light-induced polaron magnetization in EuTe at temperatures reaching 150 K

    NASA Astrophysics Data System (ADS)

    Henriques, A. B.; Galgano, G. D.; Rappl, P. H. O.; Abramof, E.

    2016-05-01

    We demonstrate that light creates a highly magnetized region in a magnetic semiconductor far above its critical temperature. A near-gap photon generates a quasiparticle of nonzero magnetic moment, named magnetic polaron, which is constituted by the photoexcited electron and about 1000 spin-polarized lattice atoms surrounding the photoexcited electron. The photoinduced magnetization follows a Langevin function, whose shape uniquely determines the magnetic moment of an individual polaron. In EuTe at 5 K the magnetic moment reaches a giant value of over 500 Bohr magnetons, thus the photoinduced magnetization saturates with a magnetic field of only 50 mT, which characterizes the magnetic polaron system as superparamagnetic. The polaron has an average lifetime of 15 μ s . When temperature is increased its magnetic moment decreases, but at 150 K it still has a large value of about 80 Bohr magnetons. The paramagnet of polarons is fully controlled by light. Because the magnetic polaron affects only spin orientation, but not the charge distribution, in the superparamagnetic state the ideal optical quality of the host semiconductor is preserved.

  19. A magnetic polaron model for the enhanced Curie temperature of EuO(1-x).

    PubMed

    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.

  20. Luminescence properties of magnetic polarons in EuTe: Theoretical description and experiments in magnetic fields up to 28 T

    NASA Astrophysics Data System (ADS)

    Henriques, A. B.; Moraes, F. C. D.; Galgano, G. D.; Meaney, A. J.; Christianen, P. C. M.; Maan, J. C.; Abramof, E.; Rappl, P. H. O.

    2014-10-01

    The recent discovery of a polaron-associated zero phonon line in the band-edge photoluminescence of high optical quality EuTe crystals opens up the prospect of answering long-standing questions about the polaron internal structure, thermal stability, and generation efficiency. Here, a Schrödinger equation for the polaron was formulated and resolved by using both variational and self-consistent methods. The theory is in good agreement with measurements of the zero phonon line as a function of magnetic field and temperature, and it could be applied to other polaronic systems. It is deduced that, in EuTe, at 0K, a polaron carries a magnetic moment of 610μB, and its binding energy is 27 meV. However, this binding energy does not carry the usual meaning of thermal stability, because it decreases drastically when the sample is warmed up. For instance, at T =100K, the binding energy is already reduced to only 6 meV. The thermal destruction of a polaron is brought about by thermal fluctuations of the spin lattice that suppress the electron's self-energy. Photoluminescence excitation spectra of EuTe demonstrate that the photogeneration of polarons becomes increasingly inefficient when the energy of the pumping photon is increased above the band gap.

  1. Quantitative measurements of magnetic polaron binding on acceptors in CdMnTe alloys

    NASA Astrophysics Data System (ADS)

    Nhung, Tran Hong; Planel, R.

    1983-03-01

    The acceptor binding energy is measured as a function of Temperature and composition in Cd1-x Mnx Te alloys, by time resolved spectroscopy. The Bound magnetic polaron effect is measured and compared with a theory accouting for magnetic saturation and fluctuations.

  2. Time-resolved magnetophotoluminescence studies of magnetic polaron dynamics in type-II quantum dots

    NASA Astrophysics Data System (ADS)

    Barman, B.; Oszwałdowski, R.; Schweidenback, L.; Russ, A. H.; Pientka, J. M.; Tsai, Y.; Chou, W.-C.; Fan, W. C.; Murphy, J. R.; Cartwright, A. N.; Sellers, I. R.; Petukhov, A. G.; Žutić, I.; McCombe, B. D.; Petrou, A.

    2015-07-01

    We used continuous wave photoluminescence (cw-PL) and time-resolved photoluminescence (TR-PL) spectroscopy to compare the properties of magnetic polarons (MP) in two related spatially indirect II-VI epitaxially grown quantum dot systems. In the ZnTe /(Zn ,Mn )Se system the holes are confined in the nonmagnetic ZnTe quantum dots (QDs), and the electrons reside in the magnetic (Zn,Mn)Se matrix. On the other hand, in the (Zn ,Mn )Te /ZnSe system, the holes are confined in the magnetic (Zn,Mn)Te QDs, while the electrons remain in the surrounding nonmagnetic ZnSe matrix. The magnetic polaron formation energies EMP in both systems were measured from the temporal redshift of the band-edge emission. The magnetic polaron exhibits distinct characteristics depending on the location of the Mn ions. In the ZnTe /(Zn ,Mn )Se system the magnetic polaron shows conventional behavior with EMP decreasing with increasing temperature T and increasing magnetic field B . In contrast, EMP in the (Zn ,Mn )Te /ZnSe system has unconventional dependence on temperature T and magnetic field B ; EMP is weakly dependent on T as well as on B . We discuss a possible origin for such a striking difference in the MP properties in two closely related QD systems.

  3. Bound Polaron Pair Formation in Poly (phenylenevinylenes)

    NASA Astrophysics Data System (ADS)

    Rothberg, Lewis

    The following sections are included: * INTRODUCTION * PHOTOGENERATED YIELD OF SINGLET EXCITONS * AGGREGRATION EFFECTS ON EXCITED STATE PHOTO-GENERATION * ASSIGNMENT TO BOUND POLARON PAIRS AND DISCUSSION * PROBLEMS WITH THE BOUND POLARON PAIR PICTURE AND CONCLUSION * REFERENCES

  4. Optical orientation of hole magnetic polarons in (Cd,Mn)Te/(Cd,Mn,Mg)Te quantum wells

    NASA Astrophysics Data System (ADS)

    Zhukov, E. A.; Kusrayev, Yu. G.; Kavokin, K. V.; Yakovlev, D. R.; Debus, J.; Schwan, A.; Akimov, I. A.; Karczewski, G.; Wojtowicz, T.; Kossut, J.; Bayer, M.

    2016-06-01

    The optically induced spin polarization in (Cd,Mn)Te/(Cd,Mn,Mg)Te diluted-magnetic-semiconductor quantum wells is investigated by means of picosecond pump-probe Kerr rotation. At 1.8 K temperature, additionally to the oscillatory signals from photoexcited electrons and manganese spins precessing about an external magnetic field, a surprisingly long-lived (up to 60 ns) nonoscillating spin polarization is detected. This polarization is related to optical orientation of equilibrium magnetic polarons involving resident holes. The suggested mechanism for the optical orientation of the equilibrium magnetic polarons indicates that the detected polaron dynamics originates from unexcited magnetic polarons. The polaron spin dynamics is controlled by the anisotropic spin structure of the heavy hole resulting in a freezing of the polaron magnetic moment in one of the two stable states oriented along the structure growth axis. Spin relaxation between these states is prohibited by a potential barrier, which depends on temperature and magnetic field. The magnetic polaron relaxation is accelerated with increasing temperature and in magnetic field.

  5. Polaron-like vortices, dissociation transition, and self-induced pinning in magnetic superconductors

    SciTech Connect

    Bulaevskii, L. N. Lin, S.-Z.

    2013-09-15

    Vortices in magnetic superconductors polarize spins nonuniformly and repolarize them when moving. At a low spin relaxation rate and at low bias currents, vortices carrying magnetic polarization clouds become polaron-like and their velocities are determined by the effective drag coefficient that is significantly bigger than the Bardeen-Stephen (BS) one. As the current increases, vortices release polarization clouds and the velocity as well as the voltage in the I-V characteristics jump to values corresponding to the BS drag coefficient at a critical current J{sub c}. The nonuniform components of the magnetic field and magnetization drop as the velocity increases, resulting in weaker polarization and a discontinuous dynamic dissociation depinning transition. Experimentally, the jump shows up as a depinning transition and the corresponding current at the jump is the depinning current. As the current decreases, on the way back, vortices are retrapped by polarization clouds at the current J{sub r} < J{sub c}. As a result, the polaronic effect suppresses dissipation and enhances the critical current. Borocarbides (RE)Ni{sub 2}B{sub 2}C with a short penetration length and highly polarizable rare earth spins seem to be optimal systems for a detailed study of vortex polaron formation by measuring I-V characteristics. We also propose to use a superconductor-magnet multilayer structure to study polaronic mechanism of pinning with the goal to achieve high critical currents. The magnetic layers should have large magnetic susceptibility to enhance the coupling between vortices and magnetization in magnetic layers while the relaxation of the magnetization should be slow. For Nb and a proper magnet multilayer structure, we estimate the critical current density J{sub c} {approx} 10{sup 9} A/m{sup 2} at the magnetic field B Almost-Equal-To 1 T.

  6. New Models of Magnetic Interactions for Bound Magnetic Polarons in Dilute Magnetic Semiconductors

    NASA Astrophysics Data System (ADS)

    McIntyre, Cynthia R.

    The goal of the first part of this thesis is to develop a solvable model that better approximates the true exchange Hamiltonian of bound magnetic polarons (BMPs). The model replaces the single exchange constant (one-step) of the previous model by two exchange parameters (two-steps) of different coupling strengths. This formulation of the Hamiltonian breaks up some of the degeneracy of the one -step model. Determination of the relevant parameters is done using a Feynman (17) variational method. This method gives the optimal values for parameters in the model. A comparison of parameters, significant to the one-step model, using Feynman's variational method and a technique by Ryabchenko (14) will be presented. The second part of this thesis will focus on the effects of anisotropic exchange interaction, Dzyaloshinski (15) -Moriya (16) (DM) interaction, on the magnetization of the dilute magnetic semiconductors. Anisotropic exchange (DM) is the largest of the known non-spin conserving interactions. Because of its non-spin conserving property, anisotropic exchange is a probable mechanism for affecting the magnetization of Mn^{+2} pairs. Recent experimental research (22) on these materials has focused on the contribution of the DM interaction at the energy level crossings of Mn^{+2} pairs. We calculate the contribution of DM to the magnetization and compare to the linewidth of magnetization steps obtained from experiment. Also, we theoretically investigate the role of spin-lattice interactions on the relaxation of Mn^{+2} pairs and compare the theoretical time to the estimated experimental time (22). (Copies available exclusively from MIT Libraries, Rm. 14-0551, Cambridge, MA 02139-4307. Ph. 617-253-5668; Fax 617-253-1690.) (Abstract shortened with permission of school.).

  7. 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.

  8. 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.

  9. 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.

  10. 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

  11. Magnetic field tuning of polaron losses in Fe doped BaTiO3 single crystals

    NASA Astrophysics Data System (ADS)

    Anand Theerthan, R.; Artemenko, Alla; Maglione, Mario

    2012-10-01

    Artificial tuning of dielectric parameters can result from interface conductivity in polycrystalline materials. In ferroelectric single crystals, it has already been shown that ferroelectric domain walls can be the source of such artificial coupling. We show here that low-temperature dielectric losses can be tuned by a dc magnetic field. Since such losses were previously ascribed to polaron relaxation we suggest this results from the interaction of hopping polarons with the magnetic field. The fact that this loss alteration has no counterpart in the real part of the dielectric permittivity confirms that no interface is involved in this purely dynamical effect. The contribution of mobile charges hopping among Fe-related centers was confirmed by ESR spectroscopy, showing a maximum intensity at ca T ˜ 40 K.

  12. 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.

  13. Photogeneration of Polarons in Sexithiophene Oligomers

    NASA Astrophysics Data System (ADS)

    Ehrenfreund, Eitan

    1996-03-01

    We present photoexcitation studies of vacuum deposited neutral films of sexithiophene (6T) using photoinduced absorption spectroscopy and photoinduced absorption detected magnetic resonance (PADMR) techniques. We find evidence for photoinduced polarons (photoexcited ``radical ions'') having spin 1/2, with two absorption bands at 0.80 and 1.54 eV, respectively, and with negative PADMR signal at g~=2. Similar absorption bands are observed in lightly p-doped sexithiophene, and are interpreted as due to 6T^ -- + radical cations. In addition, a photoinduced absorption band is found at ~=1.1 eV, which is shorter lived and decreases faster with increasing temperature than the polaron bands. We identify this band as due to spinless bipolarons (photoexcited ``di-ions''). A similar di-cation (6T^++) band has been identified in heavily p-doped sexithiophene. Each of the polaron and bipolaron peaks, observed here, is accompanied by a secondary shoulder on its low energy side. This observation may indicate a possible breaking of charge conjugation symmetry, with negatively charged polarons (bipolarons) having lower energy transitions than positively charged polarons (bipolarons). Finally, we have identified triplet excitons (S=1) with triplet-triplet transition energy at ~=1.45 eV. Work done in collaboration with J. Poplawski (Technion), X. Wei, P. Lane and Z.V. Vardeny (University of Utah, Salt Lake City, UT), M. Ibrahim and A.J. Frank (NREL, Golden, CO). Supported by the US--Israel Binational Science Foundation (BSF 94--256).

  14. The conversion of the small magnetic polarons into the large polaron as the cause of the unusual transport properties of layered manganites La1.2Sr1.8Mn2O7

    NASA Astrophysics Data System (ADS)

    Solin, N. I.

    2016-03-01

    The paper is aimed at clarification of nature of unusual transport properties of the layered manganites. Magnetic and magnetotransport properties of the Mn-deficient quasi-two-dimensional manganites La1,2Sr1,8Mn2(1-z)O7 are investigated at 5-400 K in magnetic fields up to 9 T. The studied single crystals show properties typical to layered manganites. Semiconductor-metal-like transition near the Curie temperature (TC), non-metal type of resistance ρ(T) at low temperatures, enormous magnetoresistance near TC, the negative magnetoresistance in the studied temperature range are observed in these single crystals. The obtained results are discussed in the framework of the magnetic polaron conductivity. It is assumed that in quasi-two-dimensional manganites the polarons are preserved in the magnetically ordered state as well, and that small magnetic polarons become big polaron at low temperatures. The increase of size of the magnetic polaron under magnetic ordering or application of a magnetic field explains the basic transport properties of layered manganites La1.2Sr1.8Mn2O7. The temperature and field dependencies of the polaron sizes, defined from the magnetotransport properties, are reasonably described in the model of phase separation.

  15. Magnetic control of Coulomb scattering and terahertz transitions among excitons

    NASA Astrophysics Data System (ADS)

    Bhattacharyya, J.; Zybell, S.; Eßer, F.; Helm, M.; Schneider, H.; Schneebeli, L.; Böttge, C. N.; Breddermann, B.; Kira, M.; Koch, S. W.; Andrews, A. M.; Strasser, G.

    2014-03-01

    Time-resolved terahertz quenching studies of the magnetoexcitonic photoluminescence from GaAs/AlGaAs quantum wells are performed. A microscopic theory is developed to analyze the experiments. Detailed experiment-theory comparisons reveal a remarkable magnetic-field controllability of the Coulomb and terahertz interactions in the excitonic system.

  16. Exciton effective mass enhancement in coupled quantum wells in electric and magnetic fields

    NASA Astrophysics Data System (ADS)

    Wilkes, J.; Muljarov, E. A.

    2016-02-01

    We present a calculation of exciton states in semiconductor coupled quantum wells in the presence of electric and magnetic fields applied perpendicular to the QW plane. The exciton Schrödinger equation is solved in real space in three-dimensions to obtain the Landau levels of both direct and indirect excitons. Calculation of the exciton energy levels and oscillator strengths enables mapping of the electric and magnetic field dependence of the exciton absorption spectrum. For the ground state of the system, we evaluate the Bohr radius, optical lifetime, binding energy and dipole moment. The exciton mass renormalization due to the magnetic field is calculated using a perturbative approach. We predict a non-monotonous dependence of the exciton ground state effective mass on magnetic field. Such a trend is explained in a classical picture, in terms of the ground state tending from an indirect to a direct exciton with increasing magnetic field.

  17. Magnetic-field-induced nonparabolicity of exciton dispersion in semiconductors with a nondegenerate valence band

    SciTech Connect

    Loginov, D. K. Chegodaev, A. D.

    2011-09-15

    The nonparabolicity of exciton dispersion due to the mixing of the ground and excited states of an exciton in an external magnetic field perpendicular to the direction of its motion is considered. A model describing this effect is proposed and the nonparabolicity for an exciton in a CdTe crystal is calculated. The magnetic-field induced exciton nonparabolicity is compared with the effect caused by the nonparabolicity of the electron energy dispersion in the conduction band.

  18. Dynamics of photogenerated polarons in conjugated polymers.

    PubMed

    An, Z; Wu, C Q; Sun, X

    2004-11-19

    Within a tight-binding electron-phonon interacting model, we investigate the dynamics of photoexcitations to address the generation mechanism of charged polarons in conjugated polymers by using a nonadiabatic evolution method. Besides the neutral polaron exciton which is well known, we identify a novel product of lattice dynamic relaxation from the photoexcited states in a few hundreds of femtoseconds, which is a mixed state composed of both charged polarons and neutral excitons. Our results show that the charged polarons are generated directly with a yield of about 25%, which is independent of the excitation energies, in good agreement with results from experiments. Effects of the conjugation length are also discussed.

  19. Dynamics of Photogenerated Polarons in Conjugated Polymers

    NASA Astrophysics Data System (ADS)

    An, Z.; Wu, C. Q.; Sun, X.

    2004-11-01

    Within a tight-binding electron-phonon interacting model, we investigate the dynamics of photoexcitations to address the generation mechanism of charged polarons in conjugated polymers by using a nonadiabatic evolution method. Besides the neutral polaron exciton which is well known, we identify a novel product of lattice dynamic relaxation from the photoexcited states in a few hundreds of femtoseconds, which is a mixed state composed of both charged polarons and neutral excitons. Our results show that the charged polarons are generated directly with a yield of about 25%, which is independent of the excitation energies, in good agreement with results from experiments. Effects of the conjugation length are also discussed.

  20. Magnetic Brightening of Dark Excitons in Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Kono, Junichiro

    2007-03-01

    To gain insight into the internal energy structure and radiative properties of excitons in single-walled carbon nanotubes (SWNTs), we have studied photoluminescence (PL) from individualized HiPco and CoMoCAT samples as a function of magnetic field (B) and temperature (T). The PL intensity increased, or ``brightened,'' with B applied along the tube axis and the amount of brightening increased with decreasing T. These results are consistent with the existence of a dark state below the first bright state [1]. In the presence of time reversal symmetry, exchange-interaction-induced mixing between excitons in two equivalent valleys (the K and K' valleys) is expected to result in a set of exciton states, only one of which is optically active. This predicted bright state, however, is not the lowest in energy. Excitons would be trapped in the dark, lowest-energy state without a radiative recombination path. When a tube-threading B is applied, addition of an Aharonov-Bohm phase modifies the circumferential boundary conditions on the wave functions and lifts time reversal symmetry [2,3]. This symmetry breaking splits the K and K' valley transitions, lessening the intervalley mixing and causing the recovery of the unmixed direct K and K' excitons, which are both optically active. We have calculated PL spectra through B-dependent effective masses, populations of finite-k states, and acoustic phonon scattering, which quantitatively agree with the observations. These results demonstrate the existence of dark excitons, their influence on the PL quantum yield, and their elimination through symmetry manipulation by a B. This work was performed in collaboration with J. Shaver, S. Zaric, O. Portugall, V. Krstic, G. L. J. A. Rikken, X. Wei, S. A. Crooker, Y. Miyauchi, S. Maruyama, and V. Perebeinos and supported by the Robert A. Welch Foundation, the NSF, and EuroMagNET. [1] V. Perebeinos et al., Phys. Rev. Lett. 92, 257402 (2004); H. Zhao and S. Mazumdar, Phys. Rev. Lett. 93, 157402

  1. Bethe-Salpeter equation for exciton states in quantum well in a nonhomogeneous magnetic field

    NASA Astrophysics Data System (ADS)

    Koinov, Z.; Nash, P.; Witzel, J.

    2003-03-01

    The trapping of excitons in a single quantum well due to the presence of an external strong constant magnetic field and a small nonhomogeneous cylindrical symmetric magnetic field, created by a magnetized disk on top of the quantum well, is studied by applying the Bethe-Salpeter formalism. The numerical calculations are performed for GaAs/AlGaAs quantum wells. We find that the nonhomogeneous magnetic field leads to the formation of bound exciton states with nonzero values for the center-of-mass exciton wave function only in a sufficiently small area.

  2. Bethe-Salpeter equation for quantum-well exciton states in an inhomogeneous magnetic field

    NASA Astrophysics Data System (ADS)

    Koinov, Z. G.; Nash, P.; Witzel, J.

    2003-04-01

    The trapping of excitons in a single quantum well due to the presence of a strong homogeneous magnetic field and a weak inhomogeneous cylindrical symmetric magnetic field, created by the deposition of a magnetized disk on top of the quantum well, both applied perpendicular to the x-y plane of confinement is studied theoretically. The numerical calculations are performed for GaAs/AlxGa1-xAs quantum wells and the formation of bound exciton states with nonzero values for the center-of-mass exciton wave function only in a small area is predicted.

  3. Simultaneous monitoring of singlet and triplet exciton variations in solid organic semiconductors driven by an external static magnetic field

    SciTech Connect

    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.

  4. Analytical method for determining quantum well exciton properties in a magnetic field

    NASA Astrophysics Data System (ADS)

    Stépnicki, Piotr; Piétka, Barbara; Morier-Genoud, François; Deveaud, Benoît; Matuszewski, Michał

    2015-05-01

    We develop an analytical approximate method for determining the Bohr radii of Wannier-Mott excitons in thin quantum wells under the influence of magnetic field perpendicular to the quantum well plane. Our hybrid variational-perturbative method allows us to obtain simple closed formulas for exciton binding energies and optical transition rates. We confirm the reliability of our method through exciton-polariton experiments realized in a GaAs/AlAs microcavity with an 8 nm InxGa1 -xAs quantum well and magnetic field strengths as high as 14 T.

  5. Optically detected magnetic resonance (ODMR) studies of fullerene-doped pi-conjugated polymers

    NASA Astrophysics Data System (ADS)

    Shinar, Joseph; Lane, P. A.

    1995-12-01

    The X-band photoluminescence (PL) and PL-detected magnetic resonance (PLDMR) of C60- and C70-doped pristine 2,5-dihexoxy poly(p-phenylene vinylene) (DHOPPV), poly(3-dodecyl thiophene) (P3DT), and 2,5-dibutoxy poly(p-phenylene ethynylene) (DBOPPE) are described and discussed. While light (approximately 0.1 mol.%) doping of pristine DHOPPV sharply weakens the PL, it strongly enhances the PL-enhancing polaron and triplet exciton resonances, which are very weak in the undoped film. The polaron PLDMR is attributed to magnetic resonance enhancement of nonradiative trapped polaron pair recombination, which reduces the polaron population and consequently the rate at which they nonradiatively quench singlet excitons. Its behavior in 0.1 mol.% C60:DHOPPV is discussed in relation to the potential effects of C60-counterions, including the photogeneration of trapped polaron pairs at the expense of singlet excitons, and the fission of singlet excitons to such pairs. The emergence of the triplet resonance is discussed in relation to intersystem crossing from the singlet to the triplet manifold induced by the C60 dopant. At higher doping levels, the polaron and triplet exciton resonances weaken with increasing C60 content. The reduced polaron resonance is discussed in relation to the smaller relative change in the polaron population at the field for resonance, and the potential effects of the dissociation of the polaron pairs. The behavior of C70-doped pristine DHOPPV at up to 1 mol.% C70 is qualitatively similar to that of C60: DHOPPV, but the polaron resonance in P3DT and DBOPPE is less sensitive to C60. The triplet resonance is almost completely suppressed even in lightly doped P3DT and DBOPPE, which is attributed to quenching by the injected polarons.

  6. Ground state energy of an exciton in a spherical quantum dot in the presence of an external magnetic field

    SciTech Connect

    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.

  7. 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 CO 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.

  8. Excitonic magnetism in Van Vleck-type d4 Mott insulators.

    PubMed

    Khaliullin, Giniyat

    2013-11-01

    In Mott insulators with the t(2g)4 electronic configuration such as of Re3+, Ru4+, Os4+, and Ir5+ ions, spin-orbit coupling dictates a Van Vleck-type nonmagnetic ground state with an angular momentum J=0, and the magnetic response is governed by gapped singlet-triplet excitations. We derive the exchange interactions between these excitons and study their collective behavior on different lattices. In perovskites, a conventional Bose condensation of excitons into a magnetic state is found, while an unexpected one-dimensional behavior supporting spin-liquid states emerges in honeycomb lattices, due to the bond directional nature of exciton interactions in the case of 90° d-p-d bonding geometry.

  9. Vector polarons in a degenerate electron system

    NASA Astrophysics Data System (ADS)

    Clougherty, Dennis P.; Foell, Charles A.

    2004-08-01

    We consider a one-dimensional model of an electron in a doubly (or nearly) degenerate band that interacts with elastic distortions. We show that the electron equations of motion reduce to a set of coupled nonlinear Schrödinger equations. For the case of interband electron-phonon coupling stemming from local Jahn-Teller interactions, multicomponent self-localized polaron solutions-vector polarons- are described and classified. The phase diagram for the different types of vector polarons in this model is presented. By interpreting the components of the orbital doublet as those of spin- (1)/(2) , our results can also be used to describe bound magnetic polarons.

  10. Tunable Magnetic Alignment between Trapped Exciton-Polariton Condensates

    NASA Astrophysics Data System (ADS)

    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.

    2016-03-01

    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.

  11. Tunable Magnetic Alignment between Trapped Exciton-Polariton Condensates.

    PubMed

    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.

  12. Influence of a spin-orbit exciton on the magnetic ordering in Sr2IrO4

    NASA Astrophysics Data System (ADS)

    Dikushina, E. A.; Avvakumov, I. L.

    2016-09-01

    This study investigates a spin-orbit exciton propagation in quasi-two-dimensional Heisenberg antiferromagnet Sr2IrO4 by means of computer simulations. Heisenberg model is used with consideration of magnetic interactions and exciton hopping. As the result of this simulation spin structure factor and dynamic spin structure factor are calculated.

  13. Excitonic diamagnetic shifts and linewidths in Al_xGa_1-xAs alloys in high magnetic fields

    NASA Astrophysics Data System (ADS)

    Senger, R. T.; Coli, G.; Bajaj, K. K.; Reno, J. L.; Jones, E. D.; Crooker, Scott

    2002-03-01

    We have measured both the diamagnetic shifts and the linewidths of excitonic transitions in Alx Ga_1-xAs alloys as a function of aluminum concentration and magnetic field at 1.4 K using photoluminescence spectroscopy. The aluminum composition in our samples ranged from 0 to 300 to 50 tesla. The samples were grown on GaAs substrates oriented along [001] direction using molecular beam epitaxy at 590ºC. We find that for a given value of alloy composition, both the diamagnetic shift and excitonic linewidth increase as a function of magnetic field. The observed variations of the diamagnetic shifts and excitonic linewidths with magnetic field are considerably smaller than those calculated by Lee and Bajaj [J. Appl. Phys. 73, 1788 (1993)] using a free exciton model. To explain our experimental data we propose that the excitons are localized in a very specific manner. To simulate exciton localization, we assume that the exciton reduced mass is increased and is obtained by using the alloy dependent heavy-hole mass along [001] direction treated isotropically. The calculated values of the variations of the diamagnetic shift and excitonic linewidth as a function of magnetic field obtained using this model agree very well with those reported here. Sandia is a multiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy under contract DE-AC04-94AL85000.

  14. Effect of carrier doping on the formation and collapse of magnetic polarons in lightly hole-doped La1-xSrxCoO3

    SciTech Connect

    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.

  15. {sup 139}La NMR in lanthanum manganites: Indication of the presence of magnetic polarons from spectra and nuclear relaxations

    SciTech Connect

    Allodi, G.; De Renzi, R.; Guidi, G.

    1998-01-01

    We present {sup 139}La NMR experiments on five powder samples of lanthanum manganites, with a Mn{sup 4+} concentration ranging from the antiferromagnetic-insulator (AFM) to the ferromagnetic-conducting (FM) region of the phase diagram. We measure a positive hyperfine coupling C=0.13 T/{mu}{sub B}. A signal from nuclei in a FM environment is present at all compositions, as evidenced by a hyperfine frequency in zero-field experiments, by a positive hyperfine shift in NMR experiments below T{sub c}, and by a paramagnetic frequency shift following Curie-Weiss law. A signal from nuclei in an AFM environment is identified by a similar negative intercept Curie-Weiss law. The NMR spectra reveal a large temperature dependent fraction of static spin defects below T{sub c} in the FM domains. Nuclear relaxation indicates that the FM regions are influenced by diffusing, AFM-correlated excitations, while the AFM regions probe spin fluctuations from diffusing, FM correlated excitations. These results are interpreted in terms of electronic inhomogeneities due to the presence of a magnetic small polaron. {copyright} {ital 1998} {ital The American Physical Society}

  16. Polarons in π-Conjugated Polymers: Anderson or Landau?

    PubMed

    Barford, William; Marcus, Max; Tozer, Oliver Robert

    2016-02-01

    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.

  17. Highly accurate analytical energy of a two-dimensional exciton in a constant magnetic field

    NASA Astrophysics Data System (ADS)

    Hoang, Ngoc-Tram D.; Nguyen, Duy-Anh P.; Hoang, Van-Hung; Le, Van-Hoang

    2016-08-01

    Explicit expressions are given for analytically describing the dependence of the energy of a two-dimensional exciton on magnetic field intensity. These expressions are highly accurate with the precision of up to three decimal places for the whole range of the magnetic field intensity. The results are shown for the ground state and some excited states; moreover, we have all formulae to obtain similar expressions of any excited state. Analysis of numerical results shows that the precision of three decimal places is maintained for the excited states with the principal quantum number of up to n=100.

  18. Evidence for photogenerated intermediate hole polarons in ZnO

    NASA Astrophysics Data System (ADS)

    Sezen, Hikmet; Shang, Honghui; Bebensee, Fabian; Yang, Chengwu; Buchholz, Maria; Nefedov, Alexei; Heissler, Stefan; Carbogno, Christian; Scheffler, Matthias; Rinke, Patrick; Wöll, Christof

    2015-04-01

    Despite their pronounced importance for oxide-based photochemistry, optoelectronics and photovoltaics, only fairly little is known about the polaron lifetimes and binding energies. Polarons represent a crucial intermediate step populated immediately after dissociation of the excitons formed in the primary photoabsorption process. Here we present a novel approach to studying photoexcited polarons in an important photoactive oxide, ZnO, using infrared (IR) reflection-absorption spectroscopy (IRRAS) with a time resolution of 100 ms. For well-defined (10-10) oriented ZnO single-crystal substrates, we observe intense IR absorption bands at around 200 meV exhibiting a pronounced temperature dependence. On the basis of first-principles-based electronic structure calculations, we assign these features to hole polarons of intermediate coupling strength.

  19. Evidence for photogenerated intermediate hole polarons in ZnO.

    PubMed

    Sezen, Hikmet; Shang, Honghui; Bebensee, Fabian; Yang, Chengwu; Buchholz, Maria; Nefedov, Alexei; Heissler, Stefan; Carbogno, Christian; Scheffler, Matthias; Rinke, Patrick; Wöll, Christof

    2015-04-22

    Despite their pronounced importance for oxide-based photochemistry, optoelectronics and photovoltaics, only fairly little is known about the polaron lifetimes and binding energies. Polarons represent a crucial intermediate step populated immediately after dissociation of the excitons formed in the primary photoabsorption process. Here we present a novel approach to studying photoexcited polarons in an important photoactive oxide, ZnO, using infrared (IR) reflection-absorption spectroscopy (IRRAS) with a time resolution of 100 ms. For well-defined (10-10) oriented ZnO single-crystal substrates, we observe intense IR absorption bands at around 200 meV exhibiting a pronounced temperature dependence. On the basis of first-principles-based electronic structure calculations, we assign these features to hole polarons of intermediate coupling strength.

  20. Evidence for photogenerated intermediate hole polarons in ZnO.

    PubMed

    Sezen, Hikmet; Shang, Honghui; Bebensee, Fabian; Yang, Chengwu; Buchholz, Maria; Nefedov, Alexei; Heissler, Stefan; Carbogno, Christian; Scheffler, Matthias; Rinke, Patrick; Wöll, Christof

    2015-01-01

    Despite their pronounced importance for oxide-based photochemistry, optoelectronics and photovoltaics, only fairly little is known about the polaron lifetimes and binding energies. Polarons represent a crucial intermediate step populated immediately after dissociation of the excitons formed in the primary photoabsorption process. Here we present a novel approach to studying photoexcited polarons in an important photoactive oxide, ZnO, using infrared (IR) reflection-absorption spectroscopy (IRRAS) with a time resolution of 100 ms. For well-defined (10-10) oriented ZnO single-crystal substrates, we observe intense IR absorption bands at around 200 meV exhibiting a pronounced temperature dependence. On the basis of first-principles-based electronic structure calculations, we assign these features to hole polarons of intermediate coupling strength. PMID:25902307

  1. Charge-transfer excitons in DNA.

    PubMed

    Conwell, E M; McLaughlin, P M; Bloch, S M

    2008-02-21

    There have been a number of theoretical treatments of excitons in DNA, most neglecting both the intrachain and interchain wavefunction overlaps of the electron and hole, treating them as Frenkel excitons. Recently, the importance of the intrachain and interchain coupling has been highlighted. Experiments have shown that in (dA)n oligomers and in duplex (dA)n.(dT)n, to be abbreviated (A/T), where A is adenine and T is thymine, the exciton wavefunction is delocalized over several bases. In duplexes it is possible to have charge-transfer (CT) excitons. Theoretical calculations have suggested that CT excitons in DNA may have lower energy than single chain excitons. In all the calculations of excitons in DNA, the polarization of the surrounding water has been neglected. Calculations have shown, however, that polarization of the water by an excess electron or a hole in DNA lowers its energy by approximately 1/2 eV, causing it to become a polaron. It is therefore to be expected that polarization charge induced in the surrounding water has a significant effect on the properties of the exciton. In what follows, we present calculations of some properties CT excitons would have in an A/T duplex taking into account the wavefunction overlaps, the effect of the surrounding water, which results in the electron and hole becoming polarons, and the ions in the water. As expected, the CT exciton has lowest energy when the electron and hole polarons are directly opposite each other. By appropriate choice of the dielectric constant, we can obtain a CT exciton delocalized over the number of sites found in photoinduced absorption experiments. The absorption threshold that we then calculate for CT exciton creation in A/T is in reasonable agreement with the lowest singlet absorption deduced from available data. PMID:18232682

  2. Photogeneration of polaron pairs in conducting polymers

    NASA Astrophysics Data System (ADS)

    Conwell, E. M.; Mizes, H. A.

    1995-03-01

    It is usually assumed that when photogeneration in a conducting polymer results in an electron and hole on separate chains they form negative and positive polarons that can move independently of each other. We show, on the basis of the small carrier yield per photon seen in picosecond photoconductivity, the different behavior of photoinduced absorption (PA) in dilute solution and thin films, and the spectral distribution of the PA in thin films, that photogenerated positive and negative polarons in poly(p-phenylene vinylene), polythiophene, and polyacetylene are, for the most part, bound in pairs by their Coulomb attraction. We also show that PA data give evidence for a gap of 2.8 eV, and thus an exciton binding energy of 0.4 eV, in poly(p-phenylene vinylene).

  3. Magnetic field effects on the Rabi splitting and radiative decay rates of the exciton-polariton states in a semiconductor microcavity

    NASA Astrophysics Data System (ADS)

    Fenniche, H.; Jaziri, S.; Bennaceur, R.

    1998-12-01

    We study theoretically a particular type of semiconductor microcavity formed by a quantum well embedded inside it and the distributed Bragg reflectors presenting a gradual structure. We apply to this structure a static magnetic field along the growth direction. In the strong coupling regime between the confined exciton and cavity modes, we evaluate the polariton Rabi splitting corresponding to the two lowest lying exciton states: HH1-CB1 and HH2-CB2 as a function of the applied magnetic field. In high magnetic field and for distinct reflectivities, we find that the Rabi splitting magnitude of the HH2-CB2 exciton is close to the fundamental one (HH1-CB1). In the presence of the magnetic field, the polariton Rabi splitting can be obtained even in low reflectivity. The dispersion polariton radiative decay rates related to the two lowest lying exciton states: HH1-CB1 and HH2-CB2 are calculated for different magnetic field values. At k //=0 and in the weak coupling regime, the polariton radiative decay rates are evaluated for both the HH1-CB1 and HH2-CB2 excitons. We show that for the fundamental excitonic state, the magnetic field value which determines the transition from the weak to the strong coupling regime is different from the HH2-CB2 exciton state.

  4. Robust ground state and artificial gauge in DQW exciton condensates under weak magnetic field

    NASA Astrophysics Data System (ADS)

    Hakioğlu, T.; Özgün, Ege; Günay, Mehmet

    2014-08-01

    An exciton condensate is a vast playground in studying a number of symmetries that are of high interest in the recent developments in topological condensed matter physics. In double quantum wells (DQWs) they pose highly nonconventional properties due to the pairing of non-identical fermions with a spin dependent order parameter. Here, we demonstrate a new feature in these systems: the robustness of the ground state to weak external magnetic field and the appearance of the artificial spinor gauge fields beyond a critical field strength where negative energy pair-breaking quasi particle excitations, i.e. de-excitation pockets (DX-pockets), are created in certain k regions. The DX-pockets are the Kramers symmetry broken analogs of the negative energy pockets examined in the 1960s by Sarma. They respect a disk or a shell-topology in k-space or a mixture between them depending on the magnetic field strength and the electron-hole density mismatch. The Berry connection between the artificial spinor gauge field and the TKNN number is made. This field describes a collection of pure spin vortices in real space when the magnetic field has only inplane components.

  5. Polarons in acetanilide

    SciTech Connect

    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.

  6. Polarons in acetanilide

    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.

  7. 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.

  8. Localized and bound excitons in type-II ZnMnSe/ZnSSe quantum wells.

    PubMed

    Chernenko, A V; Brichkin, A S

    2014-10-22

    Photoluminescence of ZnMnSe/ZnSSe multiple quantum wells under a bandgap continuous wave and fs-pulsed excitations is measured in magnetic fields up to 10 T in Faraday geometry at temperatures within the range of 1.6-20 K. The measurements reveal two dominant lines in the spectra and LO-phonon replicas of the lower-energy line. The photoluminescence and time-resolved studies show dramatically different behaviour of the lines. Analysis of their properties reveals that they correspond to recombination of indirect localized excitons and indirect acceptor-bound excitons (A0X). Crossing of exciton and A0X lines because of the difference in magnitudes of their Zeeman shifts is observed. Analysis of LO-phonon replicas of photoluminescence lines provides additional evidence for strong carrier localization bound to A0X. A model of phonon-assisted recombination of indirect acceptor-bound excitons is proposed. The fitting of photoluminescence lines with this model gives the Huang-Rhys factor S≃0.25 for A0X and the hole localization size ah≃30 Å. Contrary to expectations the exciton magnetic polaron effect is hardly observed in these structures. PMID:25273841

  9. Phase diagram of a spinor exciton-polariton condensate in a disordered microcavity in the presence of a magnetic field

    SciTech Connect

    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.

  10. Dynamics of exciton recombination in strong magnetic fields in ultrathin GaAs/AlAs quantum wells with indirect band gap and type-II band alignment

    NASA Astrophysics Data System (ADS)

    Shamirzaev, T. S.; Debus, J.; Yakovlev, D. R.; Glazov, M. M.; Ivchenko, E. L.; Bayer, M.

    2016-07-01

    The exciton recombination dynamics is studied experimentally and theoretically in two-monolayer-thick GaAs/AlAs quantum wells characterized by an indirect band gap and a type-II band alignment. At cryogenic temperatures, the lifetimes of the excitons that are indirect both in real and k space are in the millisecond range. The exciton recombination time and the photoluminescence (PL) intensity are strongly dependent on strength and orientation of an applied magnetic field. In contrast to the very weak influence of an in-plane field, at 2 K temperature a field applied parallel to the growth axis drastically slows down the recombination and reduces the PL intensity. With increasing temperature the magnetic field effects on PL intensity and decay time are vanishing. The experimental data are well described by a model for the exciton dynamics that takes into account the magnetic-field-induced redistribution of the indirect excitons between their bright and dark states. It allows us to evaluate the lower bound of the heavy-hole longitudinal g factor of 2.5, the radiative recombination time for the bright excitons of 0.34 ms, and the nonradiative recombination time of the bright and dark excitons of 8.5 ms.

  11. Role of triplet polaron pairs in conjugated polymer photophysics

    NASA Astrophysics Data System (ADS)

    Wesely, Elizabeth; Rothberg, Lewis; Marchetti, Alfred; Chen, Shaw; Geng, Yanhou; Culligan, Sean

    2007-03-01

    We measure the decay of the long-lived fluorescence of a conjugated oligofluorene at temperatures from 300 K to 20 K. We conclude that nearly all of this emission arises from geminate recombination of photogenerated polaron pairs to reform the singlet exciton, and that charge pair recombination represents a significant contribution to the overall fluorescence quantum yield. The unusual nonmonotonic decay dynamics of the delayed fluorescence can be explained if we assume interconversion between singlet and triplet polaron pairs on the submicrosecond time scale. (˜500 ns.) We are able to model the decay of the delayed fluorescence by assuming activated recombination from a Gaussian energy distribution of singlet polaron pairs centered 0.2 eV below the excited state and having a standard deviation of 0.12 eV. The model is relevant to recent work involving the measurement of singlet-triplet branching ratios and to the yields of electroluminescent devices.

  12. Defects-assisted ferromagnetism due to bound magnetic polarons in Ce into Fe, Co:ZnO nanoparticles and first-principle calculations.

    PubMed

    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. PMID:26831598

  13. "Watching" Polaron Pair Formation from First-Principles Electron-Nuclear Dynamics.

    PubMed

    Donati, Greta; Lingerfelt, David B; Petrone, Alessio; Rega, Nadia; Li, Xiaosong

    2016-09-22

    The formation of polaron pairs is one of the important photophysical processes that take place after the excitation in semiconducting organic polymers. First-principles Ehrenfest excited-state dynamics is a unique tool to investigate ultrafast photoinduced charge carrier dynamics and related nonequilibrium processes involving correlated electron-nuclear dynamics. In this work the formation of polaron pairs and their dynamical evolution in an oligomer of seven thiophene units is investigated with a combined approach of first-principles exciton-nuclear dynamics and wavelet analysis. The real-time formation of a polaron pair can be observed in the dipole evolution during the excited-state dynamics. The possible driving force of the polaron pair formation is investigated through qualitative correlation between the structural dynamics and the dipole evolution. The time-dependent characteristics and spectroscopic consequences of the polaron pair formation are probed using the wavelet analysis. PMID:27571540

  14. Exciton spin dynamics and photoluminescence polarization of CdSe/CdS dot-in-rod nanocrystals in high magnetic fields

    NASA Astrophysics Data System (ADS)

    Siebers, B.; Biadala, L.; Yakovlev, D. R.; Rodina, A. V.; Aubert, T.; Hens, Z.; Bayer, M.

    2015-04-01

    The exciton spin dynamics and polarization properties of the related emission are investigated in colloidal CdSe/CdS dot-in-rod (DiR) and spherical core/shell nanocrystal (NC) ensembles by magneto-optical photoluminescence (PL) spectroscopy in magnetic fields up to 15 T. It is shown that the degree of circular polarization (DCP) of the exciton emission induced by the magnetic field is affected by the NC geometry as well as the exciton fine structure and can provide information on nanorod orientation. A theory to describe the circular and linear polarization properties of the NC emission in a magnetic field is developed. It takes into account phonon mediated coupling between the exciton fine structure states as well as the dielectric enhancement effect resulting from the anisotropic shell of DiR NCs. This theoretical approach is used to model the experimental results and allows us to explain most of the measured features. The spin dynamics of the dark excitons is investigated in magnetic fields by time-resolved photoluminescence. The results highlight the importance of confined acoustic phonons in the spin relaxation of dark excitons. The bare core surface as well as the core/shell interface give rise to an efficient spin-relaxation channel, while the surface of core/shell NCs seems to play only a minor role.

  15. Role of photogenerated meta-stable polarons in organic magnetoresistance: evidence for polaron pair mechanism

    NASA Astrophysics Data System (ADS)

    Gautam, Bhoj; Nguyen, Tho; Valy Vardeny, Z.

    2010-03-01

    We studied the magneto-conductance (MC) in homopolar organic diodes based on semiconductor polymers MEH-PPV and DOO-PPV. In dark we measured negative MC in both MEH-PPV and DOO-PPV homopolar devices, which was previously interpreted as due to magnetic field effect on singlet yield of polaron pairs having the same charge, known in the literature as the ``bipolaron'' mechanism. We investigated the role of photogenerated meta-stable polarons on the MC, when illuminating the device with a cw laser beam at various intensities and illumination times. Such illumination is known to produce metastable polarons that are deep-trapped in MEH-PPV polymer, but less so in DOO-PPV polymer. Upon illumination we obtained a gradual change in the MC magnitude and magnetic field response, where the MC first decreases then changes sign from negative to positive with the illumination time. Similar effects were not obtained in DOO-PPV devices. We therefore conclude that the metastable polarons in the illuminated polymer initiate the formation of polaron pairs with opposite charge in the homopolar device upon current injection; and these are therefore responsible for positive MC. This photoinduced MC is in agreement with a similar effect found in MC of bipolar organic diodes upon increasing the bias voltage beyond the threshold for bipolar injection.

  16. 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.

  17. Dynamics of exciton dissociation in donor-acceptor polymer heterojunctions.

    PubMed

    Sun, Zhen; Stafström, Sven

    2013-04-28

    Exciton dissociation in a donor-accepter polymer heterojunction has been simulated using a nonadiabatic molecular dynamics approach, which allows for the coupled evolution of the nuclear degrees of freedom and the electronic degrees of freedom described by multiconfigurational electronic wavefunctions. The simulations reveal important details of the charge separation process: the exciton in the donor polymer first dissociates into a "hot" charge transfer state, which is best described as a polaron pair. The polaron pair can be separated into free polaron charge carriers if a sufficiently strong external electric field is applied. We have also studied the effects of inter-chain interaction, temperature, and the external electric field strength. Increasing inter-chain interactions makes it easier for the exciton to dissociate into a polaron pair state, but more difficult for the polaron pair to dissociate into free charge carriers. Higher temperature and higher electric field strength both favor exciton dissociation as well as the formation of free charge carriers. PMID:23635169

  18. Polaronic effects at finite temperatures in the B850 ring of the LH2 complex.

    PubMed

    Chorošajev, Vladimir; Rancova, Olga; Abramavicius, Darius

    2016-03-21

    Energy transfer and relaxation dynamics in the B850 ring of LH2 molecular aggregates are described, taking into account the polaronic effects, by a stochastic time-dependent variational approach. We explicitly include the finite temperature effects in the model by sampling the initial conditions of the vibrational states randomly. This is in contrast to previous applications of the variational approach, which consider only the zero-temperature case. The method allows us to obtain both the microscopic dynamics at the single-wavefunction level and the thermally averaged picture of excitation relaxation over a wide range of temperatures. Spectroscopic observables such as temperature dependent absorption and time-resolved fluorescence spectra are calculated. Microscopic wavefunction evolution is quantified by introducing the exciton participation (localization) length and the exciton coherence length. Their asymptotic temperature dependence demonstrates that the environmental polaronic effects range from exciton self-trapping and excitonic polaron formation at low temperatures to thermally induced state delocalization and decoherence at high temperatures. While the transition towards the polaronic state can be observed on the wavefunction level, it does not produce a discernible effect on the calculated spectroscopic observables.

  19. Bipolar polaron pair recombination in polymer/fullerene solar cells

    NASA Astrophysics Data System (ADS)

    Kupijai, Alexander J.; Behringer, Konstantin M.; Schaeble, Florian G.; Galfe, Natalie E.; Corazza, Michael; Gevorgyan, Suren A.; Krebs, Frederik C.; Stutzmann, Martin; Brandt, Martin S.

    2015-12-01

    We present a study of the rate-limiting spin-dependent charge-transfer processes in different polymer/fullerene bulk-heterojunction solar cells at 10 K . Observing central spin-locking signals in pulsed electrically detected magnetic resonance and an inversion of Rabi oscillations in multifrequency electron-double-resonance spectroscopy, we find that the spin response of both spin-coated and printed P3HT/PCBM and spin-coated PCDTBT/PCBM solar cells at low temperatures is governed by bipolar polaron pair recombination and quantitatively determine the polaron-polaron coupling strength with double electron-electron resonance experiments. Furthermore spin Hahn echo decay and inversion recovery measurements are performed to measure spin coherence and recombination times of the polaron pairs, respectively.

  20. Photophysics of the geminate polaron-pair state in copper phthalocyanine organic photovoltaic blends: evidence for enhanced intersystem crossing.

    PubMed

    Snedden, Edward W; Monkman, Andrew P; Dias, Fernando B

    2013-04-01

    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.

  1. Sub-picosecond spin relaxation of bright excitons and imbalance suppression in asymmetric Cdse/Zns nanocrystal quantum dots under an applied magnetic field.

    PubMed

    Kyhm, Kwangseuk; Kim, Jihoon; Yang, Ho-Soon; Je, Koo-Chul; Murayama, Akihiro

    2012-03-01

    The ultrafast spin dynamics of the bright exciton in CdSe/ZnS nanocrystal quantum dots has been investigated using a circularly polarized pump-probe experiment. A remarkably fast spin flip (-500 fs) of the bright exciton was observed at 4 K, which is attributed to the anisotropic electron-hole exchange interaction and the random positioning of nanocrystal quantum dots. In the presence of an applied magnetic field (5 T), the exciton spin parallel to the external magnetic field was favored due to Zeeman splitting. We found that this imbalance can possibly be suppressed by the state-blocking and the mixing of the 1(L) and 1(U) states in asymmetric quantum dots.

  2. Magnetic field control of the neutral and charged exciton fine structure in single quantum dashes emitting at 1.55 μm

    SciTech Connect

    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.

  3. Excitons in coupled type-II double quantum wells under electric and magnetic fields: InAs/AlSb/GaSb

    SciTech Connect

    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.

  4. Role of amorphous and aggregate phases on field-induced exciton dissociation in a conjugated polymer

    NASA Astrophysics Data System (ADS)

    Mróz, Marta M.; Lüer, Larry; Houarner-Rassin, Coralie; Anderson, Harry L.; Cabanillas-Gonzalez, Juan

    2013-01-01

    We have applied electric field assisted pump-probe spectroscopy in order to unravel the interplay of amorphous and aggregate phases on the polaron-pair photogeneration process in a conjugated porphyrin polymer. We find that excitons photogenerated in both phases are precursors for polaron pairs with different yields. Kinetic modeling indicates a substantially larger barrier for exciton dissociation in aggregates compared to amorphous areas. The majority of polaron pairs are however formed in aggregate phases due to efficient energy transfer from the amorphous phase. Based on the change in the Stark shift associated with the photogenerated polaron density, we provide a picture of the motion of polaron pairs under the external electric field.

  5. Origin of the Efficient Polaron-Pair Dissociation in Polymer-Fullerene Blends

    NASA Astrophysics Data System (ADS)

    Deibel, Carsten; Strobel, Thomas; Dyakonov, Vladimir

    2009-07-01

    The separation of photogenerated polaron pairs in organic bulk heterojunction solar cells is the intermediate but crucial step between exciton dissociation and charge transport to the electrodes. In state-of-the-art devices, above 80% of all polaron pairs are separated at fields of below 107V/m. In contrast, considering just the Coulomb binding of the polaron pair, electric fields above 108V/m would be needed to reach similar yields. In order to resolve this discrepancy, we performed kinetic Monte Carlo simulations of polaron-pair dissociation in donor-acceptor blends, considering delocalized charge carriers along conjugated polymer chain segments. We show that the resulting fast local charge carrier transport can indeed explain the high experimental quantum yields in polymer solar cells.

  6. Origin of the efficient polaron-pair dissociation in polymer-Fullerene blends.

    PubMed

    Deibel, Carsten; Strobel, Thomas; Dyakonov, Vladimir

    2009-07-17

    The separation of photogenerated polaron pairs in organic bulk heterojunction solar cells is the intermediate but crucial step between exciton dissociation and charge transport to the electrodes. In state-of-the-art devices, above 80% of all polaron pairs are separated at fields of below 10(7) V/m. In contrast, considering just the Coulomb binding of the polaron pair, electric fields above 10(8) V/m would be needed to reach similar yields. In order to resolve this discrepancy, we performed kinetic Monte Carlo simulations of polaron-pair dissociation in donor-acceptor blends, considering delocalized charge carriers along conjugated polymer chain segments. We show that the resulting fast local charge carrier transport can indeed explain the high experimental quantum yields in polymer solar cells.

  7. 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.

  8. Effective Masses of Vector Polarons

    NASA Astrophysics Data System (ADS)

    Foell, Charles; Clougherty, Dennis

    2006-03-01

    We consider the vector polarons of a one-dimensional model of an electron in a doubly (or nearly) degenerate band that couples to two elastic distortions, as described previously by Clougherty and Foell [1]. A variational approach is used to analytically and numerically calculate effective masses of the three types of vector polarons. [1] D. P. Clougherty and C. A. Foell, Phys. Rev. B 70, 052301 (2004).

  9. Monotonicity of the Polaron Energy

    NASA Astrophysics Data System (ADS)

    Miyao, Tadahiro

    2014-12-01

    In condensed matter physics, the polaron is described by the Hamiltonian of H. Fröhlich. In this paper, the Fröhlich Hamiltonian is investigated from a viewpoint of operator inequalities proposed in [36]. This point of view clarifies the monotonicity of polaron energy, i.e. denoting the lowest energy of the Fröhlich Hamiltonian with the ultraviolet cutoff Λ by EΛ, we prove that EΛ, >EΛ‧ for Λ < Λ‧.

  10. Non-canonical distribution and non-equilibrium transport beyond weak system-bath coupling regime: A polaron transformation approach

    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.

  11. 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

  12. Criteria for the accuracy of small polaron quantum master equation in simulating excitation energy transfer dynamics

    SciTech Connect

    Chang, Hung-Tzu; Cheng, Yuan-Chung; Zhang, Pan-Pan

    2013-12-14

    The small polaron quantum master equation (SPQME) proposed by Jang et al. [J. Chem. Phys. 129, 101104 (2008)] is a promising approach to describe coherent excitation energy transfer dynamics in complex molecular systems. To determine the applicable regime of the SPQME approach, we perform a comprehensive investigation of its accuracy by comparing its simulated population dynamics with numerically exact quasi-adiabatic path integral calculations. We demonstrate that the SPQME method yields accurate dynamics in a wide parameter range. Furthermore, our results show that the accuracy of polaron theory depends strongly upon the degree of exciton delocalization and timescale of polaron formation. Finally, we propose a simple criterion to assess the applicability of the SPQME theory that ensures the reliability of practical simulations of energy transfer dynamics with SPQME in light-harvesting systems.

  13. Magnetic Field Induced Charged Exciton Studies in a GaAs/Al(0.3)Ga(0.7)As Single Heterojunction

    SciTech Connect

    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/Al0.3Ga0.7As 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.

  14. Evidence of Bound Magnetic Polaron-Mediated Weak Ferromagnetism in co-doped SnO2 Nanocrystals: Microstructural, Optical, Hyperfine, and Magnetic Investigations

    NASA Astrophysics Data System (ADS)

    Inpasalini, M. S.; Choubey, Ravi Kant; Mukherjee, Samrat

    2016-07-01

    Phase-pure rutile SnO2 nanoparticles doped with various pairs of transition metals such as Fe-Ni, Fe-Mn, Ni-Mn, and Co-Mn have been synthesized using a sol-gel method. Average crystallite size of 22 nm to 29 nm with no impurity secondary phase was observed by x-ray diffraction (XRD) analysis. The morphologies of the particles were studied and their sizes calculated by field-emission scanning electron microscopy (FESEM). Emission at 338 nm in photoluminescence (PL) spectroscopy was observed and attributed to band-edge emission, while the peak at 470 nm was ascribed to doubly ionized oxygen vacancies. Raman spectroscopy confirmed the phase purity of the sample. The effects of oxygen vacancies broaden the E g mode of the Raman spectrum. In 119Sn Mössbauer spectra, broadened line width was observed and the singlet was attributed to Sn4+ valence state. The interaction between singly ionized oxygen vacancies and 3 d dopant ion is the reason behind the ferromagnetic ordering observed in magnetic studies. Spins pinned at the surface orient randomly, which decreases the total moment.

  15. Ultrafast photogeneration of charged polarons on conjugated polymer chains in dilute solution

    NASA Astrophysics Data System (ADS)

    Miranda, Paulo B.; Moses, Daniel; Heeger, Alan J.

    2004-08-01

    Ultrafast photoinduced absorption by infrared-active vibrational modes is used to study the photogeneration of polarons on semiconducting polymer chains in dilute solutions and in solid films of a soluble derivative of poly(para-phenylene vinylene). In dilute solutions, polaron pairs are photogenerated on the conjugated polymer within less than 250fs with quantum efficiencies ϕch˜3% , about one-third of that for solid films of the same polymer. The excitation spectra of ϕch for both solutions and films show that ϕch is weakly dependent on photon energy between 2.2eV (the onset of absorption) and 4.7eV . The recombination dynamics of polarons is very fast and highly dependent on the excitation density for polymer films, but it is significantly slower and less sensitive to pump intensity for the semiconducting polymer in dilute solution. We conclude that the positive and negative polarons on a single chain in solution are typically separated by hundreds of monomer repeat units and that their one-dimensional diffusion along the chain is inhibited by the intervening excitons. This, together with the suppression of interchain recombination, explains the surprisingly slower polaron recombination in isolated chains.

  16. 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

  17. Suppression of Zeeman splitting of the energy levels of exciton-polariton condensates in semiconductor microcavities in an external magnetic field.

    PubMed

    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.

  18. Magnetic Field Effects in a Correlated Electron System with Spin-State Degree of Freedom — Implications for an Excitonic Insulator —

    NASA Astrophysics Data System (ADS)

    Tatsuno, Taro; Mizoguchi, Eriko; Nasu, Joji; Naka, Makoto; Ishihara, Sumio

    2016-08-01

    Magnetic field (H) effects on a correlated electron system with a spin-state degree of freedom are examined. The effective Hamiltonian derived from the two-orbital Hubbard model is analyzed by the mean-field approximation. Applying a magnetic field to the low-spin (LS) phase induces an excitonic insulating phase as well as a spin-state ordered phase where the LS and high-spin (HS) states are ordered alternately. When H is applied to the HS phase, a reentrant transition for the HS phase appears. A rich variety of the phase diagrams is attributed to the spin-state degree of freedom and their combinations in the wave function as well as in the real-space configuration. The present results provide a possible interpretation for the recent experimental observation of LaCoO3 under a strong magnetic field.

  19. Singlet exciton fission photovoltaics.

    PubMed

    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

  20. 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.

  1. Conjugated “Molecular Wire” for Excitons

    SciTech Connect

    Shibano, Y.; Miller, J.; Imahori, H.; Sreearunothai, P.; Cook, A.R.

    2010-05-06

    We have synthesized new conjugated, rigid rod oligomers of fluorene, F{sub n}(C{sub 60}){sub 2}, n = 4, 8, 12, and 16. These pure compounds have F{sub n} chains up to 140 {angstrom} long. The C{sub 60} groups covalently attached at both ends serve as traps for excitons created in the F{sub n} chains. Excitons created in the chains by photoexcitation reacted rapidly with the C{sub 60} groups with decays described well by the sum of two exponentials. Mean reaction times were 2.3, 5.5, and 10.4 ps for n = 8, 12, and 16. In F{sub 16}(C{sub 60}){sub 2}, the 10.4 ps reaction time was 40 times faster than that found in earlier reports on molecules of slightly longer length. The simplest possible model, that of one-dimensional diffusion of excitonic polarons that react whenever they encounter the end of a chain, fits the results to obtain diffusion coefficients. Deviations of those fits from the data may point to the need for alternative pictures or may just indicate that diffusion is not ideal. The definite lengths of these molecules enable a stringent test for theories. These results reveal that exciton transport can be much faster than previously believed, a finding that could, along with appropriate nanoassembly, enable new kinds of high-efficiency organic photovoltaics.

  2. Part 1: Synthesis and characterization of magnetic chromium5tellurium nanoparticles Part 2: Local atomic structure studies using theory to simulate polarons in superconducting cuprates and experiment to analyze alternative energy nanomaterials

    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.

  3. 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.

  4. Theory of core excitons

    SciTech Connect

    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)

  5. The properties of strong couple bound polaron in monolayer graphene

    NASA Astrophysics Data System (ADS)

    Ding, Zhao-Hua; Zhao, Ying; Xiao, Jing-Lin

    2016-09-01

    Based on the Hamiltonian of the interaction energy between electron on the surface of the graphene and longitudinal acoustic phonon on the surface of the substrate, the paper studies the properties of strong couple polaron in monolayer graphene considering the coulomb doping problem. The conventional Lee-Low-Pine unitary transformation method and linear combination operator method are used to calculate the ground state energy of the polaron. The results show that the ground state energy of the system has a linear relationship with the magnetic field strength, the cut-off wave number, the coulomb bound parameter, the distance between the graphene and the substrates, meanwhile, the ground state energy will split into two branches near the Dirac point.

  6. Femtosecond study of exciton dynamics in polyfluorene statistical copolymers in solutions and thin films

    NASA Astrophysics Data System (ADS)

    Zhang, Jin Z.; Kreger, Melissa A.; Klaerner, Gerrit; Kreyenschmidt, M.; Miller, Robert D.; Scott, J. Campbell

    1997-12-01

    The formation and decay dynamics of photogenerated excitons in polyfluorene statistical co-polymers in solutions and in thin films have been studied using femtosecond transient absorption spectroscopy. In solution photoexcitation of the polymer generates primarily intrachain singlet excitons which are initially hot and then relax quickly (< 200 fs) towards the equilibrium position in the excited state. The exciton subsequently decays following a double exponential with time constants of 30 ps and 330 ps in toluene. The fast decay is attributable to vibrational relaxation, spectral diffusion, or internal conversion (recombination) of the exciton from the excited to the ground electronic state through tunneling or thermal-activated barrier crossing before thermalization. The slow decay is assigned to conversion of the thermalized exciton to the ground state through both radiative and non-radiative pathways. In films the exciton dynamics are found to depend strongly on excitation intensity. At low intensity, the dynamics are similar to that in solutions, with a double exponential decay with time constants of 15 ps and 300 ps. At high intensities, a fast decay component with a time constant of 0.8 ps appears, which becomes more dominant at higher intensities. This fast decay is attributed to exciton- exciton annihilation due to high density of excitons created. The signal in films at both low and high excitation intensities is attributable to intrachain singlet excitons, as in solution. There is no evidence for formation of interchain bound polaron pairs in films at low intensities. At high intensities, the possibility cannot be ruled out completely, especially in relation to the fast decay. If bound polaron pairs are formed as indicated by the fast decay, they must be generated as a result of interaction between excitons on different chains since they are absent at low power, an they must be created and then decay within about 1 ps.

  7. 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.

  8. Optical and Magnetic Resonance Studies of Regio-Regular and Regio-Random Poly (3-hexylthiophene)/PCBM Blends

    NASA Astrophysics Data System (ADS)

    Hukic-Markosian, Golda; Zhang, Ye; Singh, Sanjeev; Vardeny, Valy

    2010-03-01

    Regio-regular (RR) P3HT has been successfully used as donor polymer in organic bulk heterojunction photovoltaic cells based on blends with fullerene acceptors; with power conversion efficiencies of over 6%. However, when regio-random (RR-a) P3HT is used as donor polymer in the blend, the power conversion efficiency drops to less than 0.5%. We have used various optical and magnetic resonance techniques to elucidate the charge photogeneration in the two polymer/fullerene blends. Using tunneling electron microscopy we conclude that phase separation takes place in blends based on RR P3HT but not in blends based on RR-a P3HT. Photoluminescence spectrum shows a prominent band in RR-a P3HT blend at 1.32 eV, indicating the dominance of charge transfer exciton recombination. Photoinduced absorption shows higher localization of polarons in RRa-P3HT blend, with a distinct PA band due to negative polaron on PCBM molecules. Photoinduced absorption detected magnetic resonance resolves the contributions of RR-a P3HT and PCBM as two resonances indicating positive polarons on the polymer and negative polaron on the fullerene. A model based on our experimental results will be discussed.

  9. Bose Polarons in the Strongly Interacting Regime.

    PubMed

    Hu, Ming-Guang; Van de Graaff, Michael J; Kedar, Dhruv; Corson, John P; Cornell, Eric A; Jin, Deborah S

    2016-07-29

    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 ^{87}Rb with a much lower density gas of fermionic ^{40}K 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. PMID:27517776

  10. 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.

  11. 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.

  12. 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.

  13. Orbital diamagnetic susceptibility in excitonic condensation phase

    NASA Astrophysics Data System (ADS)

    Sugimoto, Koudai; Ohta, Yukinori

    2016-08-01

    We study the orbital diamagnetic susceptibility in excitonic condensation phase using the mean-field approximation for a two-band model defined on a square lattice. We find that, in semiconductors, the excitonic condensation acquires a finite diamagnetic susceptibility due to spontaneous hybridization between the valence and the conduction bands, whereas in semimetals, the diamagnetic susceptibility in the normal phase is suppressed by the excitonic condensation. We also study the orbital diamagnetic and Pauli paramagnetic susceptibilities of Ta2NiSe5 using a two-dimensional three-band model and find that the calculated temperature dependence of the magnetic susceptibility is in qualitative agreement with experiment.

  14. Theory of exciton transfer and diffusion in conjugated polymers

    SciTech Connect

    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

  15. 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.

  16. Comments on polaron-phonon scattering theory

    NASA Astrophysics Data System (ADS)

    Tulub, A. V.

    2015-10-01

    We use the polaron state function described in terms of coupled classical and quantum fields to calculate the cross section of phonon scattering on a polaron. The value of the resonance momentum is determined by asymptotic values of several integrals. Calculating them with crystal parameters taken into account leads to bounds on the maximum value of the coupling constant. We confirm that the applicability domain of the strong-coupling approximation is near zero.

  17. 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.

  18. Localization length scales of triplet excitons in singlet fission materials

    NASA Astrophysics Data System (ADS)

    Bayliss, Sam L.; Thorley, Karl J.; Anthony, John E.; Bouchiat, Hélène; Greenham, Neil C.; Chepelianskii, Alexei D.

    2015-09-01

    We measure the dielectric confinement length scales of triplet excitons in organic semiconductors by jointly measuring their microwave-domain electric and magnetic susceptibilities. We apply this technique to characterize triplet excitons in two singlet fission materials with distinct solid-state packing and correlate the extracted localization length scales with the role of the excitonic environment. By using the magnetic susceptibility simultaneously determined through our experiments, we compare the independently extracted dielectric and spin-spin localization length scales, highlighting the role of local anisotropy on the properties of excitonic triplet states.

  19. Rate constant of exciton quenching of Ir(ppy)3 with hole measured by time-resolved luminescence spectroscopy

    NASA Astrophysics Data System (ADS)

    Oyama, Shiho; Sakai, Heisuke; Murata, Hideyuki

    2016-03-01

    We observed the quenching of tris(2-phenylpyridinato)iridium(III) [Ir(ppy)3] excitons by polarons (holes or electrons) by time-resolved photoluminescence (PL) spectroscopy to clarify the dynamics of the triplet-polaron quenching of excitons. We employed a hole-only device (HOD) and an electron-only device (EOD), where the emitting layer consists of Ir(ppy)3 doped in 4,4‧-bis(carbazol-9-yl)biphenyl. Time-resolved PL spectroscopy of the EOD and HOD were measured under a constant current density. The results showed that the excitons of Ir(ppy)3 were significantly quenched only by holes. The PL decay curves of HOD were well fitted by the biexponential function, where lifetimes (τ1 and τ2) remain unchanged but the coefficient of each exponential term depends on hole current density. From the results, we proposed a model of exciton quenching where the exciton-hole quenching area expands with increasing hole current density. On the basis of the model, the triplet-polaron quenching rate constant Kq was determined.

  20. 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.

  1. 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.

  2. Engineering Polarons at a Metal Oxide Surface.

    PubMed

    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 TiO_{2}(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. PMID:27661706

  3. Engineering Polarons at a Metal Oxide Surface.

    PubMed

    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 TiO_{2}(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.

  4. Polaron Properties in Armchair Graphene Nanoribbons.

    PubMed

    da Cunha, Wiliam F; Acioli, Paulo H; de Oliveira Neto, Pedro H; Gargano, Ricardo; E Silva, Geraldo M

    2016-07-14

    By means of a 2-D tight-binding model with lattice relaxation in a first-order expansion, we report different polaron properties depending on the armchair graphene nanoribbons width family as well as on its size. We find that representatives of the 3p+2 family do not present a polaronic-mediated charge transport. As for 3p and 3p+1 families, the polaron behavior was completely dependent on the system's width. In particular, we observed a greater degree of delocalization for broader nanoribbons; narrower nanoribbons of both families, on the contrary, typically presented a more localized polaronic-type transport. Energy levels and occupation numbers analysis are performed to rigorously assess the nature of the charge carrier. Time evolution in the scope of the Ehrenfest molecular dynamics was also carried out to confirm the collective behavior and stability of the carrier as a function of time. We were able to determine that polarons in nanoribbons of 3p family present higher mobility than those in 3p+1 nanoribbons. These results identify the transport process that takes place for each system, and they allow the prediction of the mobility of the charge carriers as a function of the structural properties of the system, thus providing guidance on how to improve the efficiency of graphene nanoribbon-based devices. PMID:26918483

  5. Plasmon-Polaron Coupling in Conjugated Polymer on Infrared Nanoantennas.

    PubMed

    Wang, Zilong; Zhao, Jun; Frank, Bettina; Ran, Qiandong; Adamo, Giorgio; Giessen, Harald; Soci, Cesare

    2015-08-12

    We propose and demonstrate a novel type of coupling between polarons in a conjugated polymer and localized surface plasmons in infrared (IR) nanoantennas. The near-field interaction between plasmons and polarons is revealed by polarized photoinduced absorption measurements, probing mid-IR polaron transitions, and infrared-active vibrational modes of the polymer, which directly gauge the density of photogenerated charge carriers. This work proves the possibility of tuning the polaronic properties of organic semiconductors with plasmonic nanostructures.

  6. Polarons and solitons in Jahn Teller systems

    NASA Astrophysics Data System (ADS)

    Clougherty, Dennis P.

    2007-07-01

    Using a semiclassical continuum model of an electron in a deformable molecular crystal, some properties of multicomponent generalizations of the polaron - "vector polarons" - are elucidated. Analytical solutions for the case of two electronic bands coupled to two vibrational modes are given in detail. Within the model considered, the vector polaron can be classified by its wavefunction into several types and can have features that include: (1) a spatial variation in the electronic and vibrational character, and (2) low-energy internal degrees of freedom. For the case of electronic and vibrational degeneracy, local Jahn-Teller interactions can also lead to a novel spatiotemporal soliton, a long-lived excited state of the many-electron system stabilized by the conservation law resulting from degeneracy.

  7. POLARON DYNAMICS. Long-lived photoinduced polaron formation in conjugated polyelectrolyte-fullerene assemblies.

    PubMed

    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. PMID:26089510

  8. POLARON DYNAMICS. Long-lived photoinduced polaron formation in conjugated polyelectrolyte-fullerene assemblies.

    PubMed

    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.

  9. Real Space Imaging of Spin Polarons in Zn-Doped SrCu2(BO3)2

    NASA Astrophysics Data System (ADS)

    Yoshida, M.; Kobayashi, H.; Yamauchi, I.; Takigawa, M.; Capponi, S.; Poilblanc, D.; Mila, F.; Kudo, K.; Koike, Y.; Kobayashi, N.

    2015-02-01

    We report on the real space profile of spin polarons in the quasi-two-dimensional frustrated dimer spin system SrCu2(BO3)2 doped with 0.16% of Zn. The 11B nuclear magnetic resonance spectrum exhibits 15 additional boron sites near nonmagnetic Zn impurities. With the help of exact diagonalizations of finite clusters, we have deduced from the boron spectrum, the distribution of local magnetizations at the Cu sites with fine spatial resolution, providing direct evidence for an extended spin polaron. The results are confronted with those of other experiments performed on doped and undoped samples of SrCu2(BO3)2.

  10. Additional evidence for complex 2-site polarons in CMR manganites.

    NASA Astrophysics Data System (ADS)

    Bridges, Frank; Kurczveil, Geza; Downward, Lisa; Neumeier, John J.

    2007-03-01

    Recently we have proposed a complex 2-site polaron model (which we call a dimeron) that exists for temperatures near and above the ferromagnetic transition temperature, Tc [1]. The dimeron has a hole delocalized over two Mn sites (i.e. a hole and an electron share the two Mn sites) and the two Mn sites have a reduced distortion compared to the remaining Jahn-Teller distorted electron sites. Magnetic clusters just above Tc are likely clusters of these dimeron quasiparticles. The average valance of the two Mn sites in the dimeron is 3.5 and the spin is 7/2. We show that the Mn K-absorption edge is much better described as a sum of a 3.5 valence edge (fraction 2x) plus a 3 valance edge (fraction 1-2x), compared to earlier simulations using x CaMnO3 plus 1-x LaMnO3. We also show that fitting the Mn-O peak to a sum of two experimental Mn-O standards leads to a similar result as in the earlier study - a fraction 2x of lower distorted Mn sites (dimerons) and a fraction 1-2x of more distorted sites with 1 eg electron. Both support the proposed complex - 2-site polaron model.Supported under NSF grant DMR0301971.[1] L. Downward et. al., Phys Rev Lett 95, 106401 (2005).

  11. Optically programmable excitonic traps

    PubMed Central

    Alloing, Mathieu; Lemaître, Aristide; Galopin, Elisabeth; Dubin, François

    2013-01-01

    With atomic systems, optically programmed trapping potentials have led to remarkable progress in quantum optics and quantum information science. Programmable trapping potentials could have a similar impact on studies of semiconductor quasi-particles, particularly excitons. However, engineering such potentials inside a semiconductor heterostructure remains an outstanding challenge and optical techniques have not yet achieved a high degree of control. Here, we synthesize optically programmable trapping potentials for indirect excitons of bilayer heterostructures. Our approach relies on the injection and spatial patterning of charges trapped in a field-effect device. We thereby imprint in-situ and on-demand electrostatic traps into which we optically inject cold and dense ensembles of excitons. This technique creates new opportunities to improve state-of-the-art technologies for the study of collective quantum behavior of excitons and also for the functionalisation of emerging exciton-based opto-electronic circuits. PMID:23546532

  12. Study of spin-polaron formation in 1D systems

    SciTech Connect

    Arredondo, Y.; Navarro, O.; Vallejo, E.

    2014-05-15

    We study numerically the formation of spin-polarons in low-dimensional systems. We consider a ferromagnetic Kondo lattice model with Hund coupling J{sub H} and localized spins interacting antiferromagnetically with coupling constant J. We investigate the ground state phase diagram as a function of the exchange couplings J{sub H} and J and as a function of the band filling, since it has been observed that doping either on the ferromagnetic or antiferromagnetic regime lead to formation of magnetic domains [1]. We explore the quasi-particle formation and phase separation using the density-matrix renormalization group method, which is a highly efficient method to investigate quasi-one-dimensional strongly correlated systems.

  13. One dimensional polaron effects and current inhomogeneities in sequential phonon emission

    SciTech Connect

    Hellman, E.S.; Harris, J.S.; Hanna, C.; Laughlin, R.B.

    1985-07-01

    We have constructed a physical model to explain the tunneling current oscillations reported by Hickmott et al., for GaAs/AlGaAs heterostructures in high magnetic fields. We propose that the periodic structure observed is due to space charge which builds up in the undepleted layer when electrons enter it with energy just below the phonon emission threshold. Such electrons interact with the lattice to form polarons whose energy is pinned to the phonon energy, and thus has a very small group velocity. The polaron effect is strongly enhanced by the confinement of the electrons by the strong magnetic field. We infer from the current-voltage data that most of the tunneling current flows through a small area of the sample. The combined model gives reasonable quantitative agreement with experiment. 6 refs., 6 figs.

  14. Photogenerated polarons in poly(paraphenylene vinylene)

    NASA Astrophysics Data System (ADS)

    Murata, K.; Shimoi, Y.; Abe, S.; Kuroda, S.; Noguchi, T.; Ohnishi, T.

    1998-02-01

    Photo-induced spin species in poly(paraphenylene vinylene) (PPV) and its derivative have been investigated by means of the light-induced ESR (LESR) technique using variable excitation energy. LESR spectra at the X and K bands for stretch-oriented PPV samples exhibit clear anisotropy, which is well explained in terms of the anisotropic g-value and hyperfine coupling of unpaired π electron on the conjugated chain. The X band spectra were well reproduced by theoretical ESR spectra using a polaron spin density obtained from the Pariser-Parr-Pople model. The LESR signal increases significantly above around 3 eV. This threshold is interpreted as the interband gap above which free electron-hole pairs are created efficiently. From these results, we conclude that the observed light-induced spin species are polarons.

  15. Ground state energy of large polaron systems

    SciTech Connect

    Benguria, Rafael D.; Frank, Rupert L.; Lieb, Elliott H.

    2015-02-15

    The last unsolved problem about the many-polaron system, in the Pekar–Tomasevich approximation, is the case of bosons with the electron-electron Coulomb repulsion of strength exactly 1 (the “neutral case”). We prove that the ground state energy, for large N, goes exactly as −N{sup 7/5}, and we give upper and lower bounds on the asymptotic coefficient that agree to within a factor of 2{sup 2/5}.

  16. Large magnetic field effects in electrochemically doped organic light-emitting diodes

    NASA Astrophysics Data System (ADS)

    van Reenen, S.; Kersten, S. P.; Wouters, S. H. W.; Cox, M.; Janssen, P.; Koopmans, B.; Bobbert, P. A.; Kemerink, M.

    2013-09-01

    Large negative magnetoconductance (MC) of ˜12% is observed in electrochemically doped polymer light-emitting diodes at sub-band-gap bias voltages (Vbias). Simultaneously, a positive magnetoefficiency (Mη) of 9% is observed at Vbias = 2 V. At higher bias voltages, both the MC and Mη diminish while a negative magnetoelectroluminescence (MEL) appears. The negative MEL effect is rationalized by triplet-triplet annihilation that leads to delayed fluorescence, whereas the positive Mη effect is related to competition between spin mixing and exciton formation leading to an enhanced singlet:triplet ratio at nonzero magnetic field. The resultant reduction in triplet exciton density is argued to reduce detrapping of polarons in the recombination zone at low-bias voltages, explaining the observed negative MC. Regarding organic magnetoresistance, this study provides experimental data to verify existing models describing magnetic field effects in organic semiconductors, which contribute to better understanding hereof. Furthermore, we present indications of strong magnetic field effects related to interactions between trapped carriers and excitons, which specifically can be studied in electrochemically doped organic light-emitting diodes (OLEDs). Regarding light-emitting electrochemical cells (LECs), this work shows that delayed fluorescence from triplet-triplet annihilation substantially contributes to the electroluminescence and the device efficiency.

  17. Spectrally resolved hyperfine interactions between polaron and nuclear spins in organic light emitting diodes: Magneto-electroluminescence studies

    SciTech Connect

    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.

  18. Bound Exciton Complexes

    NASA Astrophysics Data System (ADS)

    Meyer, B. K.

    In the preceding chapter, we concentrated on the properties of free excitons. These free excitons may move through the sample and hit a trap, a nonradiative or a radiative recombination center. At low temperatures, the latter case gives rise to either deep center luminescence, mentioned in Sect. 7.1 and discussed in detail in Chap. 9, or to the luminescence of bound exciton complexes (BE or BEC). The chapter continues with the most prominent of these BECs, namely A-excitons bound to neutral donors. The next aspects are the more weakly BEs at ionized donors. The Sect. 7.4 treats the binding or localization energies of BEC from a theoretical point of view, while Sect. 7.5 is dedicated to excited states of BECs, which contain either holes from deeper valence bands or an envelope function with higher quantum numbers. The last section is devoted to donor-acceptor pair transitions. There is no section devoted specifically to excitons bound to neutral acceptors, because this topic is still partly controversially discussed. Instead, information on these A0X complexes is scattered over the whole chapter, however, with some special emphasis seen in Sects. 7.1, 7.4, and 7.5.

  19. Ultrafast Dynamics of Localized and Delocalized Polaron Transitions in P3HT/PCBM Blend Materials: The Effects of PCBM Concentration

    PubMed Central

    2009-01-01

    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 (P2at 1.45 eV) and delocalized (DP2at 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. PMID:20652147

  20. Accuracy of second order perturbation theory in the polaron and variational polaron frames

    NASA Astrophysics Data System (ADS)

    Lee, Chee Kong; Moix, Jeremy; Cao, Jianshu

    2012-05-01

    In the study of open quantum systems, the polaron transformation has recently attracted a renewed interest as it offers the possibility to explore the strong system-bath coupling regime. Despite this interest, a clear and unambiguous analysis of the regimes of validity of the polaron transformation is still lacking. Here we provide such a benchmark, comparing second order perturbation theory results in the original untransformed frame, the polaron frame, and the variational extension with numerically exact path integral calculations of the equilibrium reduced density matrix. Equilibrium quantities allow a direct comparison of the three methods without invoking any further approximations as is usually required in deriving master equations. It is found that the second order results in the original frame are accurate for weak system-bath coupling; the results deteriorate when the bath cut-off frequency decreases. The full polaron results are accurate for the entire range of coupling for a fast bath but only in the strong coupling regime for a slow bath. The variational method is capable of interpolating between these two methods and is valid over a much broader range of parameters.

  1. Small polaron effect on carrier recombination in perovskite manganite thin films

    NASA Astrophysics Data System (ADS)

    Wu, G.-R.; Sasaki, M.; Isa, T.; Negishi, H.; Inoue, M.; Gao, W.-X.; Xiong, G.-C.

    2001-05-01

    Photoinduced 'transient thermoelectric effect (TTE)' in perovskite manganite La 0.6Ca 0.4MnO 3 thin film has been measured under magnetic fields. The fast decay process of TTE signals is due to a recombination of photogenerated electron-hole pairs through Mn 4+ ions as capture centers, whose evaluated cross section σ obeys the power law σ∝ T- n ( n=0.75) in the ferromagnetic phase far below Tc and in the paramagnetic phase. From the observed relaxation time τ1, we evaluated the parameter α characterizing a small polaron effect and the effective mass m∗; both are enhanced appreciably near Tc. Such anomaly is attributed to the change in the thermal velocity of diffusing holes with downspin due to a small polaron effect.

  2. Excitonic surface lattice resonances

    NASA Astrophysics Data System (ADS)

    Humphrey, A. D.; Gentile, M. J.; Barnes, W. L.

    2016-08-01

    Electromagnetic resonances are important in controlling light at the nanoscale. The most studied such resonance is the surface plasmon resonance that is associated with metallic nanostructures. Here we explore an alternative resonance, the surface exciton-polariton resonance, one based on excitonic molecular materials. Our study is based on analytical and numerical modelling. We show that periodic arrays of suitable molecular nanoparticles may support surface lattice resonances that arise as a result of coherent interactions between the particles. Our results demonstrate that excitonic molecular materials are an interesting alternative to metals for nanophotonics; they offer the prospect of both fabrication based on supramolecular chemistry and optical functionality arising from the way the properties of such materials may be controlled with light.

  3. Permanent Rabi oscillations in coupled exciton-photon systems with PT-symmetry.

    PubMed

    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.

  4. Permanent Rabi oscillations in coupled exciton-photon systems with PT -symmetry

    PubMed Central

    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

  5. Permanent Rabi oscillations in coupled exciton-photon systems with PT -symmetry

    NASA Astrophysics Data System (ADS)

    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.

  6. Nonlinear lattice relaxation of photogenerated charge-transfer excitation in halogen-bridged mixed-valence metal complexes. II. Polaron channel

    NASA Astrophysics Data System (ADS)

    Mishima, A.; Nasu, K.

    1989-03-01

    The one-dimensional extended Peierls-Hubbard model with half-filled-band electrons is studied in order to clarify the lattice relaxation path of the photogenerated charge-transfer excitation in halogen-bridged mixed-valence metal complexes. The ground and excited states are calculated within mean-field theory for electrons and the adiabatic approximation for phonons. It is concluded that the main origin of the photoinduced absorption is a distant pair of the hole-polaron and the electron-polaron. This distant pair is created not from the ground state of the self-trapped exciton (STE), but from the excited states of the STE through their autodissociation. This is consistent with the experiment on the excitation energy dependence of the photoinduced absorption yield.

  7. Size dependent polaronic conduction in hematite

    NASA Astrophysics Data System (ADS)

    Sharma, Monika; Banday, Azeem; Murugavel, Sevi

    2016-05-01

    Lithium Ion Batteries have been attracted as the major renewable energy source for all portable electronic devices because of its advantages like superior energy density, high theoretical capacity, high specific energy, stable cycling and less memory effects. Recently, α-Fe2O3 has been considered as a potential anode material due to high specific capacity, low cost, high abundance and environmental benignity. We have synthesized α-Fe2O3 with various sizes by using the ball milling and sol-gel procedure. Here, we report the dc conductivity measurement for the crystallite size ranging from 15 nm to 50nm. It has been observed that the enhancement in the polaronic conductivity nearly two orders in magnitude while reducing the crystallite size from bulk into nano scale level. The enhancement in the conductivity is due to the augmented to compressive strain developed in the material which leads to pronounced decrease in the hopping length of polarons. Thus, nanocrystaline α-Fe2O3 may be a better alternative anode material for lithium ion batteries than earlier reported systems.

  8. 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.

  9. Polaronic effects in one- and two-band quantum systems

    NASA Astrophysics Data System (ADS)

    Yin, Tao; Cocks, Daniel; Hofstetter, Walter

    2015-12-01

    In this work, we study the formation and dynamics of polarons in a system with a few impurities in a lattice immersed in a Bose-Einstein condensate (BEC). This system has been experimentally realized using ultracold atoms and optical lattices. Here, we consider a two-band model for the impurity atoms, along with a Bogoliubov approximation for the BEC, with phonons coupled to impurities via both intraband and interband transitions. We decouple this Fröhlich-type term by an extended two-band Lang-Firsov polaron transformation using a variational method. The new effective Hamiltonian with two (polaron) bands differs from the original Hamiltonian by modified coherent transport, polaron energy shifts, and induced long-range interaction. A Lindblad master-equation approach is used to take into account residual incoherent coupling between polaron and bath. This polaronic treatment yields a renormalized interband relaxation rate compared to Fermi's golden rule. For a strongly coupled two-band Fröhlich Hamiltonian, the polaron is tightly dressed in each band and can not tunnel between them, leading to an interband self-trapping effect.

  10. Excitonic transitions in ZnO/MgZnO quantum well heterostructures

    NASA Astrophysics Data System (ADS)

    Coli, Giuliano; Bajaj, K. K.

    2001-03-01

    We present a calculation of the excitonic transition energies in ZnO/MgZnO quantum well heterostructures, including the effects of the exciton-optical phonon interaction. The results of our calculations clearly show that the use of the static screened Coulomb potential to describe the electron-hole interaction and of the polaron masses for the electron and the hole leads to a poor agreement with the available experimental data[1]. On the other hand, including the exciton-phonon interaction in the calculation of the exciton binding energies, leads to the values of the excitonic transition energies which agree very well with the recently published experimental data[1]. A critical discussion of the choice of the various physical parameters used in ZnO is also presented. This leads us to suggest a value for the heavy-hole band mass of 0.78m0 and a conduction to valence band offset ratio in the range 60/40-70/30. [1] T. Makino, C. H. Chia, N. T. Tuan, H.D. Sun, Y. Segawa, M. Kawasaki, A. Ohtomo, K. Tamura and H. Koinuma, Appl. Phys. Lett. 77, 975 (2000)

  11. Massive polarons in large-energy-gap polymers

    NASA Astrophysics Data System (ADS)

    McCall, R. P.; Ginder, J. M.; Roe, M. G.; Asturias, G. E.; Scherr, E. M.; MacDiarmid, A. G.; Epstein, A. J.

    1989-05-01

    We present evidence for the existence of defect states with large mass and low mobility in the conducting polymer polyaniline. This large-energy-gap polymer has been shown to have properties significantly different from many other conducting polymers. Photoinduced infrared absorption studies presented here are consistent with the photogeneration of charged polarons. Analysis within the amplitude mode (Peierls) formalism indicates that these polarons are massive (Mpol~60me), while use of a bond-order or Holstein polaron formalism leads to even larger estimates of Mpol.

  12. Small hole polarons in rare-earth titanates

    SciTech Connect

    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.

  13. Excitonic condensation in spatially separated one-dimensional systems

    SciTech Connect

    Abergel, D. S. L.

    2015-05-25

    We show theoretically that excitons can form from spatially separated one-dimensional ground state populations of electrons and holes, and that the resulting excitons can form a quasicondensate. We describe a mean-field Bardeen-Cooper-Schrieffer theory in the low carrier density regime and then focus on the core-shell nanowire giving estimates of the size of the excitonic gap for InAs/GaSb wires and as a function of all the experimentally relevant parameters. We find that optimal conditions for pairing include small overlap of the electron and hole bands, large effective mass of the carriers, and low dielectric constant of the surrounding media. Therefore, one-dimensional systems provide an attractive platform for the experimental detection of excitonic quasicondensation in zero magnetic field.

  14. Quantum Dynamics of Ultracold Bose Polarons.

    PubMed

    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. PMID:27661684

  15. 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.

  16. Extreme electron polaron spatial delocalization in π-conjugated materials

    PubMed Central

    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

  17. 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

  18. Tunable polaronic conduction in anatase TiO2.

    PubMed

    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

    2013-05-10

    Oxygen vacancies created in anatase TiO(2) 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. PMID:23705725

  19. 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.

  20. Exciton Storage in a Nanoscale Aharonov-Bohm Ring with Electric Field Tuning

    SciTech Connect

    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.

  1. Excitons in asymmetric quantum wells

    NASA Astrophysics Data System (ADS)

    Grigoryev, P. S.; Kurdyubov, A. S.; Kuznetsova, M. S.; Ignatiev, I. V.; Efimov, Yu. P.; Eliseev, S. A.; Petrov, V. V.; Lovtcius, V. A.; Shapochkin, P. Yu.

    2016-09-01

    Resonance dielectric response of excitons is studied for the high-quality InGaAs/GaAs heterostructures with wide asymmetric quantum wells (QWs). To highlight effects of the QW asymmetry, we have grown and studied several heterostructures with nominally square QWs as well as with triangle-like QWs. Several quantum confined exciton states are experimentally observed as narrow exciton resonances. A standard approach for the phenomenological analysis of the profiles is generalized by introducing different phase shifts for the light waves reflected from the QWs at different exciton resonances. Good agreement of the phenomenological fit to the experimentally observed exciton spectra for high-quality structures allowed us to reliably obtain parameters of the exciton resonances: the exciton transition energies, the radiative broadenings, and the phase shifts. A direct numerical solution of the Schrödinger equation for the heavy-hole excitons in asymmetric QWs is used for microscopic modeling of the exciton resonances. Remarkable agreement with the experiment is achieved when the effect of indium segregation is taken into account. The segregation results in a modification of the potential profile, in particular, in an asymmetry of the nominally square QWs.

  2. Real space imaging of spin polarons in Zn-doped SrCu(2)(BO(3))(2).

    PubMed

    Yoshida, M; Kobayashi, H; Yamauchi, I; Takigawa, M; Capponi, S; Poilblanc, D; Mila, F; Kudo, K; Koike, Y; Kobayashi, N

    2015-02-01

    We report on the real space profile of spin polarons in the quasi-two-dimensional frustrated dimer spin system SrCu(2)(BO(3))(2) doped with 0.16% of Zn. The (11)B nuclear magnetic resonance spectrum exhibits 15 additional boron sites near nonmagnetic Zn impurities. With the help of exact diagonalizations of finite clusters, we have deduced from the boron spectrum, the distribution of local magnetizations at the Cu sites with fine spatial resolution, providing direct evidence for an extended spin polaron. The results are confronted with those of other experiments performed on doped and undoped samples of SrCu(2)(BO(3))(2). PMID:25699459

  3. Attractive and repulsive Fermi polarons in two dimensions.

    PubMed

    Koschorreck, Marco; Pertot, Daniel; Vogt, Enrico; Fröhlich, Bernd; Feld, Michael; Köhl, Michael

    2012-05-31

    The dynamics of a single impurity in an environment is a fundamental problem in many-body physics. In the solid state, a well known case is an impurity coupled to a bosonic bath (such as lattice vibrations); the impurity and its accompanying lattice distortion form a new entity, a polaron. This quasiparticle plays an important role in the spectral function of high-transition-temperature superconductors, as well as in colossal magnetoresistance in manganites. For impurities in a fermionic bath, studies have considered heavy or immobile impurities which exhibit Anderson's orthogonality catastrophe and the Kondo effect. More recently, mobile impurities have moved into the focus of research, and they have been found to form new quasiparticles known as Fermi polarons. The Fermi polaron problem constitutes the extreme, but conceptually simple, limit of two important quantum many-body problems: the crossover between a molecular Bose-Einstein condensate and a superfluid with BCS (Bardeen-Cooper-Schrieffer) pairing with spin-imbalance for attractive interactions, and Stoner's itinerant ferromagnetism for repulsive interactions. It has been proposed that such quantum phases (and other elusive exotic states) might become realizable in Fermi gases confined to two dimensions. Their stability and observability are intimately related to the theoretically debated properties of the Fermi polaron in a two-dimensional Fermi gas. Here we create and investigate Fermi polarons in a two-dimensional, spin-imbalanced Fermi gas, measuring their spectral function using momentum-resolved photoemission spectroscopy. For attractive interactions, we find evidence for a disputed pairing transition between polarons and tightly bound dimers, which provides insight into the elementary pairing mechanism of imbalanced, strongly coupled two-dimensional Fermi gases. Additionally, for repulsive interactions, we study novel quasiparticles--repulsive polarons--the lifetime of which determines the

  4. Exciton-photon correlations in bosonic condensates of exciton-polaritons.

    PubMed

    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.

  5. Superlinear generation of exciton and related paramagnetism induced by forward current in a diamond p-i-n junction

    SciTech Connect

    Natori, Kenji

    2015-02-07

    The concentration of excitons generated in a high-quality diamond p-i-n junction is investigated considering the forward current characteristics of the junction. As the forward current in the junction increases, the exciton concentration increases superlinearly, contrary to the linear increases of the electron and hole concentration. This tendency suggests a superlinear increase in emission intensity due to exciton recombination. The increase rate is more radical than quadratic, in accordance with the observed increase of the integrated intensity of free exciton emission. To estimate the concentration of triplet excitons generated in the p-i-n junction, observation of the paramagnetism due to the exciton spin moment is proposed. The magnetic susceptibility superlinearly increases with the increase in the forward current, unlike any other magnetic property of the device.

  6. Ab initio Lattice Results for Fermi Polarons in Two Dimensions.

    PubMed

    Bour, Shahin; Lee, Dean; Hammer, H-W; Meißner, Ulf-G

    2015-10-30

    We investigate the attractive Fermi polaron problem in two dimensions using nonperturbative Monte Carlo simulations. We introduce a new Monte Carlo algorithm called the impurity lattice Monte Carlo method. This algorithm samples the path integral in a computationally efficient manner and has only small sign oscillations for systems with a single impurity. As a benchmark of the method, we calculate the universal polaron energy in three dimensions in the scale-invariant unitarity limit and find agreement with published results. We then present the first fully nonperturbative calculations of the polaron energy in two dimensions and density correlations between the impurity and majority particles in the limit of zero-range interactions. We find evidence for a smooth crossover transition from fermionic quasiparticle to molecular state as a function of the interaction strength. PMID:26565472

  7. X-ray emission from core excitons

    NASA Astrophysics Data System (ADS)

    Carson, R. D.; Schnatterly, S. E.

    1987-07-01

    We have observed soft x-ray emission from core excitons in several semiconductors and insulators and find that the exciton intensity is related to its binding energy. We propose an explanation for these excitons and this relationship using a Wannier model. The validity of the Wannier model is further tested by comparing our measured exciton binding energies with predicted values. We conclude that this model appears to be a good starting point in the understanding of core excitons.

  8. Momentum dependence of the excitons in pentacene

    SciTech Connect

    Roth, Friedrich; Schuster, Roman; Koenig, Andreas; Knupfer, Martin; Berger, Helmuth

    2012-05-28

    We have carried out electron energy-loss investigations of the lowest singlet excitons in pentacene at 20 K. Our studies allow to determine the full exciton band structure in the a*, b* reciprocal lattice plane. The lowest singlet exciton can move coherently within this plane, and the resulting exciton dispersion is highly anisotropic. The analysis of the energetically following (satellite) features indicates a strong admixture of charge transfer excitations to the exciton wave function.

  9. Transient electrically detected magnetic resonance spectroscopy applied to organic solar cells

    SciTech Connect

    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.

  10. Numerical simulation of photoexcited polaron states in water

    SciTech Connect

    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.

  11. Studies of exciton condensation and transport in quantum Hall bilayers

    NASA Astrophysics Data System (ADS)

    Finck, Aaron David Kiyoshi

    This thesis is a report of the transport properties of bilayer two-dimensional electron systems found in GaAs/AlGaAs double quantum well semiconductor heterostructures. When a strong perpendicular magnetic field is applied so that the total Landau filling factor is equal to one and if the two layers are close enough together, a novel quantum Hall (QH) state with strong interlayer correlations can form. This QH state is often described as an excitonic condensate, in which electrons in one layer pair with holes in the other. As neutral particles, excitons feel no Lorentz force and are not confined to the edges of the bilayer system like charged quasiparticles are. Instead, excitons are expected to be able to move freely through the bulk and even flow without any dissipation under proper conditions (i.e.,~excitonic superfluidity). Counterflow studies that directly probe the bulk verify this exciton transport in the electrically insulating interior. We also report on studies of the phase boundary between the correlated and uncorrelated phases at total Landau filling factor one as the effective interlayer separation is tuned. When both phases are fully spin polarized at high Zeeman energy, the phase transition is much broader than when the uncorrelated phase is incompletely polarized at low Zeeman energy. This suggests a possible change in the nature of the phase transition in the regime of complete spin polarization.

  12. Onset of exciton-exciton annihilation in single-layer black phosphorus

    NASA Astrophysics Data System (ADS)

    Surrente, A.; Mitioglu, A. A.; Galkowski, K.; Klopotowski, L.; Tabis, W.; Vignolle, B.; Maude, D. K.; Plochocka, P.

    2016-08-01

    The exciton dynamics in monolayer black phosphorus is investigated over a very wide range of photoexcited exciton densities using time resolved photoluminescence. At low excitation densities, the exciton dynamics is successfully described in terms of a double exponential decay. With increasing exciton population, a fast, nonexponential component develops as exciton-exciton annihilation takes over as the dominant recombination mechanism under high excitation conditions. Our results identify an upper limit for the injection density, after which exciton-exciton annihilation reduces the quantum yield, which will significantly impact the performance of light emitting devices based on single-layer black phosphorus.

  13. Superexchange coupling and electron transfer in globular proteins via polaron excitations.

    PubMed

    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.

  14. Carrier generation/recombination processes and polaron effect in perovskite manganite thin films

    NASA Astrophysics Data System (ADS)

    Wu, Guang-Ri; Inoue, Masasi; Sasaki, Minoru; Negishi, Hiroshi; Xiong, Guang-Cheng

    2000-07-01

    Pulsed-laser-induced transient thermoelectric effect (TTE) for perovskite manganite films, La 0.6Ca 0.4MnO 3 (LCMO), Pr 0.67Sr 0.33MnO 3 (PSMO), La 0.7Sr 0.3MnO 3 (LSMO), has been measured under DC electric and magnetic fields. The photoinduced TTE voltage and its sign are strongly dependent on both temperature and magnetic field, which is due to the formation of a bipolar state of photogenerated electrons and holes. It is found that Jahn-Teller and polaron effects are appreciable near the Curie temperature for the carrier recombination, in particular, for LCMO with small ionic radius of Ca 2+ ions.

  15. Deep electron and hole polarons and bipolarons in amorphous oxide

    NASA Astrophysics Data System (ADS)

    Kaviani, Moloud; Strand, Jack; Afanas'ev, Valery V.; Shluger, Alexander L.

    2016-07-01

    Amorphous (a)-HfO2 is a prototype high dielectric constant insulator with wide technological applications. Using ab initio calculations we show that excess electrons and holes can trap in a-HfO2 in energetically much deeper polaron states than in the crystalline monoclinic phase. The electrons and holes localize at precursor sites, such as elongated Hf-O bonds or undercoordinated Hf and O atoms, and the polaronic relaxation is amplified by the local disorder of amorphous network. Single electron polarons produce states in the gap at ˜2 eV below the bottom of the conduction band with average trapping energies of 1.0 eV. Two electrons can form even deeper bipolaron states on the same site. Holes are typically localized on undercoordinated O ions with average trapping energies of 1.4 eV. These results advance our general understanding of charge trapping in amorphous oxides by demonstrating that deep polaron states are inherent and do not require any bond rupture to form precursor sites.

  16. 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)

  17. Polaron mass of charge carriers in semiconductor quantum wells

    SciTech Connect

    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.

  18. Polaron Localization in Conjugated Polymers by Hybrid DFT Methods

    NASA Astrophysics Data System (ADS)

    Shao, Nan; Wu, Qin; Theorey; Computation Group Team

    2013-03-01

    Reliable application of density functional theory (DFT) to study the electronic properties of polarons remains controversial. A proper description should exhibit both the formation of a charge-localized electronic state and saturation of the polaron size for increasing oligomer length. The aim of this work is to find a proper hybrid DFT method to study the chain length related electronic properties of charged conjugated polymer system. Using oligopyrrole cations as a test case, global hybrid functionals such as BHandHLYP can show charge localization, but a well-defined polaron size does not emerge when the length of the oligomer is increased; the saturation effect was not predicted correctly. By applying 100% long-range corrected hybrid functionals, LRC-PBE, the saturation of charge distribution has been achieved, implying that the LRC-PBE is a better way to describe the spatial extent of the electronic state of polypyrrole than the conventional hybrid functionals. The tuning of the range parameter and the study of other polymer polaron systems will be discussed. Supported by Brookhaven Science Associates, LLC under Contract No. DE-AC02-98CH10886 with the U.S. Department of Energy.

  19. Polarons and Mobile Impurities Near a Quantum Phase Transition

    NASA Astrophysics Data System (ADS)

    Shadkhoo, Shahriar

    This dissertation aims at improving the current understanding of the physics of mobile impurities in highly correlated liquid-like phases of matter. Impurity problems pose challenging and intricate questions in different realms of many-body physics. For instance, the problem of ''solvation'' of charged solutes in polar solvents, has been the subject of longstanding debates among chemical physicists. The significant role of quantum fluctuations of the solvent, as well as the break down of linear response theory, render the ordinary treatments intractable. Inspired by this complicated problem, we first attempt to understand the role of non-specific quantum fluctuations in the solvation process. To this end, we calculate the dynamic structure factor of a model polar liquid, using the classical Molecular Dynamics (MD) simulations. We verify the failure of linear response approximation in the vicinity of a hydrated electron, by comparing the outcomes of MD simulations with the predictions of linear response theory. This nonlinear behavior is associated with the pronounced peaks of the structure factor, which reflect the strong fluctuations of the local modes. A cavity picture is constructed based on heuristic arguments, which suggests that the electron, along with the surrounding polarization cloud, behave like a frozen sphere, for which the linear response theory is broken inside and valid outside. The inverse radius of the spherical region serves as a UV momentum cutoff for the linear response approximation to be applicable. The problem of mobile impurities in polar liquids can be also addressed in the framework of the ''polaron'' problem. Polaron is a quasiparticle that typically acquires an extended state at weak couplings, and crossovers to a self-trapped state at strong couplings. Using the analytical fits to the numerically obtained charge-charge structure factor, a phenomenological approach is proposed within the Leggett's influence functional formalism, which

  20. Optical transition energy of magneto-polaron in a GaAs{sub 0.9}P{sub 0.1}/GaAs{sub 0.6}P{sub 0.4} quantum dot

    SciTech Connect

    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.

  1. Spin Textures of Exciton-Polaritons in a Tunable Microcavity with Large TE-TM Splitting.

    PubMed

    Dufferwiel, S; Li, Feng; Cancellieri, E; Giriunas, L; Trichet, A A P; Whittaker, D M; Walker, P M; Fras, F; Clarke, E; Smith, J M; Skolnick, M S; Krizhanovskii, D N

    2015-12-11

    We report an extended family of spin textures of zero-dimensional exciton-polaritons spatially confined in tunable open microcavity structures. The transverse-electric-transverse-magnetic (TE-TM) splitting, which is enhanced in the open cavity structures, leads to polariton eigenstates carrying quantized spin vortices. Depending on the strength and anisotropy of the cavity confining potential and of the TE-TM induced splitting, which can be tuned via the excitonic or photonic fractions, the exciton-polariton emissions exhibit either spin-vortex-like patterns or linear polarization, in good agreement with theoretical modeling.

  2. Spin Textures of Exciton-Polaritons in a Tunable Microcavity with Large TE-TM Splitting

    NASA Astrophysics Data System (ADS)

    Dufferwiel, S.; Li, Feng; Cancellieri, E.; Giriunas, L.; Trichet, A. A. P.; Whittaker, D. M.; Walker, P. M.; Fras, F.; Clarke, E.; Smith, J. M.; Skolnick, M. S.; Krizhanovskii, D. N.

    2015-12-01

    We report an extended family of spin textures of zero-dimensional exciton-polaritons spatially confined in tunable open microcavity structures. The transverse-electric-transverse-magnetic (TE-TM) splitting, which is enhanced in the open cavity structures, leads to polariton eigenstates carrying quantized spin vortices. Depending on the strength and anisotropy of the cavity confining potential and of the TE-TM induced splitting, which can be tuned via the excitonic or photonic fractions, the exciton-polariton emissions exhibit either spin-vortex-like patterns or linear polarization, in good agreement with theoretical modeling.

  3. Exciton dynamicsstudied via internal THz transitions

    SciTech Connect

    Kaindl, R.A.; Hagele, D.; Carnahan, M.A.; Lovenich, R.; Chemla,D.S.

    2003-02-26

    We employ a novel, ultrafast terahertz probe to investigatethe dynamical interplay of optically-induced excitons and unboundelectron-hole pairs in GaAs quantum wells. Resonant creation ofheavy-hole excitons induces a new low-energy oscillator linked totransitions between the internal exciton degrees of freedom. The timeresolved terahertz optical conductivity is found to be a probe wellsuited for studies of fundamental processes such as formation, relaxationand ionization of excitons.

  4. Exciton coupling in molecular crystals

    NASA Technical Reports Server (NTRS)

    Ake, R. L.

    1976-01-01

    The implications of perfect exciton coupling and molecular vibrations were investigated, as well as the effect they have on the lifetime of singlet and triplet excitons coupled in a limiting geometry. Crystalline bibenzyl, Cl4Hl4, provided a situation in which these mechanisms involving exciton coupling can be studied in the limit of perfect coupling between units due to the crystal's geometry. This geometry leads to a coupling between the two halves of the molecule resulting in a splitting of the molecular excited states. The study reported involves an experimental spectroscopic approach and begins with the purification of the bibenzyl. The principal experimental apparatus was an emission spectrometer. A closed cycle cryogenic system was used to vary the temperature of the sample between 20 K and 300 K. The desired results are the temperature-dependent emission spectra of the bibenzyl; in addition, the lifetimes and quantum yields measured at each temperature reveal the effect of competing radiationless processes.

  5. Talbot Effect for Exciton Polaritons

    NASA Astrophysics Data System (ADS)

    Gao, T.; Estrecho, E.; Li, G.; Egorov, O. A.; Ma, X.; Winkler, K.; Kamp, M.; Schneider, C.; Höfling, S.; Truscott, A. G.; Ostrovskaya, E. A.

    2016-08-01

    We demonstrate, experimentally and theoretically, a Talbot effect for hybrid light-matter waves—an exciton-polariton condensate formed in a semiconductor microcavity with embedded quantum wells. The characteristic "Talbot carpet" is produced by loading the exciton-polariton condensate into a microstructured one-dimensional periodic array of mesa traps, which creates an array of phase-locked sources for coherent polariton flow in the plane of the quantum wells. The spatial distribution of the Talbot fringes outside the mesas mimics the near-field diffraction of a monochromatic wave on a periodic amplitude and phase grating with the grating period comparable to the wavelength. Despite the lossy nature of the polariton system, the Talbot pattern persists for distances exceeding the size of the mesas by an order of magnitude. Thus, our experiment demonstrates efficient shaping of the two-dimensional flow of coherent exciton polaritons by a one-dimensional "flat lens."

  6. Talbot Effect for Exciton Polaritons.

    PubMed

    Gao, T; Estrecho, E; Li, G; Egorov, O A; Ma, X; Winkler, K; Kamp, M; Schneider, C; Höfling, S; Truscott, A G; Ostrovskaya, E A

    2016-08-26

    We demonstrate, experimentally and theoretically, a Talbot effect for hybrid light-matter waves-an exciton-polariton condensate formed in a semiconductor microcavity with embedded quantum wells. The characteristic "Talbot carpet" is produced by loading the exciton-polariton condensate into a microstructured one-dimensional periodic array of mesa traps, which creates an array of phase-locked sources for coherent polariton flow in the plane of the quantum wells. The spatial distribution of the Talbot fringes outside the mesas mimics the near-field diffraction of a monochromatic wave on a periodic amplitude and phase grating with the grating period comparable to the wavelength. Despite the lossy nature of the polariton system, the Talbot pattern persists for distances exceeding the size of the mesas by an order of magnitude. Thus, our experiment demonstrates efficient shaping of the two-dimensional flow of coherent exciton polaritons by a one-dimensional "flat lens." PMID:27610883

  7. Polaron hopping in olivine phosphates studied by nuclear resonant scattering

    NASA Astrophysics Data System (ADS)

    Tracy, Sally June

    Valence fluctuations of Fe2+ and Fe3+ were studied in a solid solution of LixFePO4 by nuclear resonant forward scattering of synchrotron x rays while the sample was heated in a diamond-anvil pressure cell. The spectra acquired at different temperatures and pressures were analyzed for the frequencies of valence changes using the Blume-Tjon model of a system with a fluctuating Hamiltonian. These frequencies were analyzed to obtain activation energies and an activation volume for polaron hopping. There was a large suppression of hopping frequency with pressure, giving an anomalously large activation volume. This large, positive value is typical of ion diffusion, which indicates correlated motions of polarons, and Li+ ions that alter the dynamics of both. In a parallel study of NaxFePO4, the interplay between sodium ordering and electron mobility was investigated using a combination of synchrotron x-ray diffraction and nuclear resonant scattering. Conventional Mossbauer spectra were collected while the sample was heated in a resistive furnace. An analysis of the temperature evolution of the spectral shapes was used to identify the onset of fast electron hopping and determine the polaron hopping rate. Synchrotron x-ray diffraction measurements were carried out in the same temperature range. Reitveld analysis of the diffraction patterns was used to determine the temperature of sodium redistribution on the lattice. The diffraction analysis also provides new information about the phase stability of the system. The temperature evolution of the iron site occupancies from the Mossbauer measurements, combined with the synchrotron diffraction results give strong evidence for a relationship between the onset of fast electron dynamics and the redistribution of sodium in the lattice. Measurements of activation barriers for polaron hopping gave fundamental insights about the correlation between electronic carriers and mobile ions. This work established that polaron-ion interactions

  8. Exciton-photon correlations in bosonic condensates of exciton-polaritons

    PubMed Central

    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

  9. Exciton Distribution between the Bright and Dark States in Single Carbon Nanotubes Studied by Magneto-Photoluminescence Spectroscopy

    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).

  10. Tunable spin-polaron state in a singly clamped semiconducting carbon nanotube

    NASA Astrophysics Data System (ADS)

    Pistolesi, F.; Shekhter, R.

    2015-07-01

    We consider a semiconducting carbon nanotube (CNT) lying on a ferromagnetic insulating substrate with one end passing the substrate and suspended over a metallic gate. We assume that the polarized substrate induces an exchange interaction acting as a local magnetic field for the electrons in the nonsuspended CNT side. Generalizing the approach of I. Snyman and Yu.V. Nazarov [Phys. Rev. Lett. 108, 076805 (2012), 10.1103/PhysRevLett.108.076805], we show that one can generate electrostatically a tunable spin-polarized polaronic state localized at the bending end of the CNT. We argue that at low temperatures manipulation and detection of the localized quantum spin state are possible.

  11. A polaron model for electron transfer in globular proteins.

    PubMed

    Chuev, G N; Lakhno, V D

    1993-07-01

    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.

  12. Polaron and bipolaron of uniaxially strained one dimensional zigzag ladder

    NASA Astrophysics Data System (ADS)

    Yavidov, B. Ya.

    2016-09-01

    An influence of the uniaxial strains in one dimensional zigzag ladder (1DZL) on the properties of polarons and bipolarons is considered. It is shown that strain changes all the parameters of the system, in particular, spectrum, existing bands and the masses of charge carriers. Numerical results obtained by taking into an account the Poisson effect clearly indicate that the properties of the (bi)polaronic system can be tuned via strain. Mass of bipolaron can be manipulated by the strain too which in turn leads to the way of tuning Bose-Einstein condensation temperature TBEC of bipolarons. It is shown that TBEC of bipolarons in strained 1DZL reasonably correlates with the values of critical temperature of superconductivity of certain perovskites.

  13. Diagrammatic Monte Carlo Method for Many-Polaron Problems

    NASA Astrophysics Data System (ADS)

    Mishchenko, Andrey S.; Nagaosa, Naoto; Prokof'ev, Nikolay

    2014-10-01

    We introduce the first bold diagrammatic Monte Carlo approach to deal with polaron problems at a finite electron density nonperturbatively, i.e., by including vertex corrections to high orders. Using the Holstein model on a square lattice as a prototypical example, we demonstrate that our method is capable of providing accurate results in the thermodynamic limit in all regimes from a renormalized Fermi liquid to a single polaron, across the nonadiabatic region where Fermi and Debye energies are of the same order of magnitude. By accounting for vertex corrections, the accuracy of the theoretical description is increased by orders of magnitude relative to the lowest-order self-consistent Born approximation employed in most studies. We also find that for the electron-phonon coupling typical for real materials, the quasiparticle effective mass increases and the quasiparticle residue decreases with increasing the electron density at constant electron-phonon coupling strength.

  14. Phase diagram of degenerate exciton systems.

    PubMed

    Lai, C W; Zoch, J; Gossard, A C; Chemla, D S

    2004-01-23

    Degenerate exciton systems have been produced in quasi-two-dimensional confined areas in semiconductor coupled quantum well structures. We observed contractions of clouds containing tens of thousands of excitons within areas as small as (10 micron)2 near 10 kelvin. The spatial and energy distributions of optically active excitons were determined by measuring photoluminescence as a function of temperature and laser excitation and were used as thermodynamic quantities to construct the phase diagram of the exciton system, which demonstrates the existence of distinct phases. Understanding the formation mechanisms of these degenerate exciton systems can open new opportunities for the realization of Bose-Einstein condensation in the solid state.

  15. Charge transport in DNA in solution: The role of polarons

    PubMed Central

    Conwell, Esther M.

    2005-01-01

    Since the discovery a decade ago of rapid photoinduced electron transfer in DNA over a distance >4 nm, a large number of experiments and theories have been advanced in the attempt to characterize the transfer, mainly of a radical cation or hole. Particularly influential experiments were carried out by Giese [Giese, B. (2000) Acc. Chem. Res. 33, 631–636] on the sequence G(A)nGGG, where G is guanine and A is adenine. These experiments were interpreted as showing that for n > 3, after the holes tunnel through the first three As, they hop onto the bridge of As, where they are localized on a single A and travel further by hopping between neighboring As. Recent experiments of Barton and coworkers [Shao, F., O'Neill, M. A. & Barton, J. K. (2004) Proc. Natl. Acad. Sci. USA 101, 17914–17919] have, however, established that the hole wavefunctions are delocalized. One of the mechanisms based on delocalized hole wavefunctions that had been investigated, both experimentally and theoretically, is transport by polarons. For one type of polaron, the properties are determined by polarization of the surrounding medium (water and ions, in this case). Theory predicts that this type of polaron is delocalized over approximately four bases in DNA. Transport by these polarons could explain the results of Giese et al. [Giese, B., Amaudrut, J., Köhler, A.-K., Spormann, M. & Wessely, S. (2001) Nature 412, 318–320], recent experimental results of O'Neill and Barton [O'Neill, M. A. & Barton, J. K. (2004) J. Am. Chem. Soc. 126, 11471–11483] concerning the size of the region over which the hole is delocalized, and other experimental observations. PMID:15956188

  16. Numerical study of polaron problem in the adiabatic limit

    NASA Astrophysics Data System (ADS)

    Marsiglio, Frank; Li, Zhou; Blois, Cindy; Baillie, Devin

    2010-03-01

    We study the polaron problem in a one dimensional chain and on a two dimensional square lattice. The models we have used are the Holstein model and the Su-Schrieffer-Heeger (SSH) model. By a variational procedure based on the Lanczos method, we are able to examine the polaron problem in the limit when the mass of the ion is very large, i.e. close to the adiabatic limit. It is known that for the Holstein model there is no phase transition [1] for any nonzero phonon energy. It is also known that for the one dimensional Holstein or SSH model there will be long range order [2] (e.g. dimerization) in the adiabatic limit at half-filling. It is then interesting to study the long range order on a two dimensional square lattice in and away from the adiabatic limit. Moreover, recent progress for the single polaron near an impurity (disorder) [3] make it an interesting problem for studying bond length disorder which can change the hopping energy in a specific direction in the Holstein model. Reference: [1] H. Lowen, Phys.Rev.B 37, 8661 (1988) [2] J.E.Hirsch and E. Frandkin, Phys. Rev. Lett. 49, 402 (1982) [3]A.S.Mishchenko et.al Phys.Rev.B 79(2009) 180301(R)

  17. 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.

  18. Topological phases and polaron physics in ultracold quantum gases

    NASA Astrophysics Data System (ADS)

    Grusdt, Fabian

    2016-05-01

    The description of quantum many-body systems poses a formidable theoretical challenge. A seemingly simple problem is the coupling of a single impurity atom to non-interacting Bogoliubov phonons in a surrounding Bose-Einstein condensate. The system can be described by a polaron model at intermediate couplings - an 80 year problem. The situation has been realized experimentally, but when the impurity mass is small compared to the Boson mass, neither mean-field nor strong-coupling expansions are valid anymore. Now the impurity acts as an exchange particle, mediating phonon-phonon interactions. In this talk I present a semi-analytical solution to the polaron problem. I will show that the approach can be generalized to solve far-from equilibrium polaron problems, too, and elaborate on connections with recent experiments involving ultracold atoms and photons. A completely different class of many-body problems are systems with topological order. In recent years we have seen an uprise of cold-atomic or photonic implementations of artificial gauge fields, providing a corner stone for the realization of topological phases of matter. In the second part of my talk, I will address the challenging problem how non-local topological orders can be detected. It will be demonstrated that many-body topological invariants can be measured, making use of mobile impurities as coherent probes of the highly entangled groundstates. I will discuss Laughlin states and comment on possible realizations using ultracold atoms.

  19. Translational mass of an exciton

    NASA Astrophysics Data System (ADS)

    Cafolla, A. A.; Schnatterly, S. E.; Tarrio, C.

    1985-12-01

    From transmission electron-energy-loss measurements we show that the mass of an exciton M* is greater than the sum of the effective masses of the electron and hole me+mh. This result is consistent with a recent prediction by Mattis and Gallinar.

  20. Exciton size and quantum transport in nanoplatelets

    SciTech Connect

    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.

  1. 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.

  2. Optical, electrical, and magnetic field studies of organic materials for light emitting diodes and photovoltaic applications

    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

  3. Interfacial and bulk polaron masses in Zn{sub 1−x}Mg{sub x}O/ZnO heterostructures examined by terahertz time-domain cyclotron spectroscopy

    SciTech Connect

    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 0.15polaron density, mass, and scattering rate. The cyclotron mass of 2D polarons was found to increase significantly with magnetic field B from 0.24 m{sub e} at B = 2 T to 0.37 m{sub e} at B = 7.5 T. A nonlinear cyclotron frequency with B was also observed for 3D polarons in ZnO. The findings are discussed in the context of polaron mass renormalization driven by the electron-LO-phonon and electron-acoustic phonon interactions.

  4. Photophysics of quasi-one-dimensional excitons in pi-conjugated polymers and semiconducting single-walled carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Sheng, Chuanxiang

    In this work we studied the ultrafast dynamics of photoexcitations in pi-conjugated organic semiconductors and semiconducting single-walled carbon nanotubes (S-NTs), using a low-intensity high-repetition rate laser system in the spectral range from 0.13 to 1.05 eV, and high-intensity low-repletion rate laser system in the spectral range from 1.2 to 2.5 eV, in the time domain from 100 fs to 1 ns. We also measured cw photomodulation (PM) spectroscopy of pi-conjugated polymers and photoluminescence (PL) spectra of both polymers and isolated nanotubes. In polymers, we found that excitons are the primary photoexcitations in single polymer chains. However, polarons and polaron pairs may also be photogenerated at early time in films. We consider this process to be extrinsic in nature, namely, dependent on materials properties, temperatures, excitation photon energies, as well as the quality of films. Both annealed and unannealed thin NT films and D2O solutions of isolated NTs were investigated. Various transient photoinduced bleaching (PB) and photoinduced absorption (PA) bands were observed, which also showed photoinduced dichroism and decay together after taking into account the PB spectral shift. The PL emission shows polarization degree. We therefore conclude that the primary photoexcitations in S-NT are excitons that are confined along the NTs. Prom the average PL polarization degree and the transient polarization memory decay, we estimate the PL lifetime in isolated NTs in solution to be of the order of 500 ps, coupling with the minute PL emission quantum efficiency, which indicates weak radiative transition strength. In S-NTs and pi-polymers, the emission spectra relative to the absorption bands are very similar, as well as transient photoinduced absorption bands (PA) with a low-energy PA1 and a higher-energy PA2 in all cases. Theoretical calculations of excited state absorptions within a correlated pi-electron Hamiltonian show the same excitonic energy spectrum

  5. Properties of a polaron confined in a spherical quantum dot

    NASA Astrophysics Data System (ADS)

    Melnikov, Dmitriy V.

    A Frohlich Hamiltonian describing the electron-phonon interaction in a spherical quantum dot embedded in another polar material is derived, taking into account interactions with both bulk longitudinal optical and surface optical phonons. The Hamiltonian is appropriate to the general case of a finite confining potential originating from a bandgap mismatch between the materials of the dot and the surrounding matrix. This Hamiltonian is then applied to treat the electron-phonon interaction in the adiabatic approximation for various quantum dot systems. It was found that, as the radius of the dot decreases, the magnitude of the electron-phonon interaction energy first increases, passes through a maximum, and then gradually decreases to the value appropriate to the situation where the electron is weakly localized inside the dot. For most dot radii the polaron properties are described well by a model assuming perfect electron confinement. Based on this result, the problem of the bound polaron confined perfectly in the quantum dot was investigated within the adiabatic and all-coupling variational approaches. The polaron properties have been studied performing both analytical and numerical calculations for various radii of the quantum dot and for different impurity positions inside the dot. Within the adiabatic approximation, it was found that the magnitude of the electron-phonon interaction increases as the radius decreases for any impurity position. It was also shown that the input from the electron-surface-phonon interaction to the total polaron energy is much larger than was found earlier for the free polaron confined in the dot. As a function of the impurity position, the electron-surface-phonon interaction energy increases as the impurity is shifted towards the surface, reaches its maximum when the impurity is positioned inside the dot and then decreases as the impurity moved close to surface. The all-coupling approach gave rise to the following results: for any

  6. Radiative recombination from dark excitons in nanocrystals: Activation mechanisms and polarization properties

    NASA Astrophysics Data System (ADS)

    Rodina, Anna V.; Efros, Alexander L.

    2016-04-01

    We analyze theoretically physical mechanisms responsible for the radiative recombination of the ground optically passive ("dark") exciton (DE), which dominates in photoluminescence (PL) of colloidal nanocrystals (NCs) at low temperatures. The DE becomes optically active due to its mixing with the bright excitons caused by an external magnetic field, dangling-bond spins or by acoustic and optical phonons. These activation mechanisms mix the DE with different bright excitons and, consequently, lead to different PL polarization properties, because they are determined by dipole orientations of the bright excitons, which the DE is coupled with. We show that the PL polarization properties of prolate and oblate shape NCs are different due to different activation mechanisms responsible for the DE recombination.

  7. Triplet excitons as sensitive spin probes for structure analysis of extended defects in microcrystalline silicon

    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 excitons reside at extended defects in the crystallites of microcrystalline silicon that give rise to shallow states in the silicon band gap. The excitons possess a rather delocalized wave function, couple to electron spins in conduction band tail states nearby, and take part in a spin-dependent recombination process. Our study shows that extended defects such as grain boundaries or stacking faults in the crystalline part of the material act as charge carrier traps that can influence the material conductivity.

  8. Spatially indirect excitons in coupled quantum wells

    SciTech Connect

    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){sup 2} were

  9. 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.

  10. Large low-symmetry polarons of the high-Tc, copper oxides: Formation, mobility and ordering

    NASA Astrophysics Data System (ADS)

    Bersuker, Gennadi I.; Goodenough, John B.

    1997-02-01

    A microscopic model of the evolution from antiferromagnetic insulator to superconductor on oxidation of the parent-phase (CuO 2) 2- sheets of a cuprate superconductor starts with the assumption that strong electron-lattice interactions are dominant and give a heterogeneous electronic distribution. Introduction of pseudo-Jahn-Teller vibronic coupling associated with the δ holes in the (CuO 2) (2-δ) - sheets is shown to stabilize, below a critical temperature Tp ≈ 850 K, large non-adiabatic polarons containing 5 to 7 copper centers; cooperative low-symmetry in-plane vibrations also stabilize an elastic attractive force between polarons that can overcome the longer-range Coulomb repulsion between polarons. Utilizing established parameters for isolated CuO 6 complexes gives a calculated polaron size of 5 to 7 copper centers, which compares with a measured mean size of 5.3 copper centers in underdoped samples 0 < δ ≤ 0.10. A large polaron is shown to move by a piece-wise tunneling of a fraction of itself across a peripheral CuO vibronic bond rather than by an activated hopping. This type of motion, which is not described by conventional transport theories, gives a linear increase of the resistivity with temperature above a temperature Tϱ due to scattering of the polaron at its own border, which separates regions inside and outside the polaron of slightly different mean CuO bond length. At lower temperatures, the polaron mobility becomes activated, but at higher concentrations this change is obscured because the elastic interpolaron attractive force causes the polarons to condense into a “polaron liquid,” and below some critical temperature Td ≥ Tc the polarons undergo long-range ordering into one-dimensional <110> polaronic stripes separated by stripes of the parent phase, which support antiferromagnetic spin fluctuations. The zig-zag polaron stripes consist of polaron pairs oriented alternately along [100] and [010] axes of a CuO 2 sheet. Formation

  11. Polaron models of high-temperature superconductivity

    NASA Astrophysics Data System (ADS)

    Mott, N. F.

    1993-01-01

    A review is given of theories of high-temperature superconductors in which the current is carried by bipolarons, which form a condensed Bose gas below Tc and a non-degenerate gas above it. Such theories were first proposed by Schafroth, Alexandrov, Ranninger and de Jongh; the present author has, for the copper oxide materials, proposed spin bipolarons. Experimental work has, however, shown no magnetic moments in the superconducting and “spin glass” ranges of composition; a modification of the spin bipolaron model is proposed to take account of these observations. Other aspects of the model are discussed, particularly heat conduction and the effect of disorder. A comparison is made with the cubic bismuth materials.

  12. Two-exciton excited states of J-aggregates in the presence of exciton-exciton annihilation

    NASA Astrophysics Data System (ADS)

    Levinsky, B.; Fainberg, B. D.; Nesterov, L. A.; Rosanov, N. N.

    2016-07-01

    We study decay of two-exciton states of a J-aggregate that is collective in nature. We use mathematical formalism based on effective non-Hermitian Hamiltonian suggested in nuclear theory. We show that decay of two-exciton states is strongly affected by the interference processes in the exciton-exciton annihilation. Our evaluations of the imaginary part of the effective Hamiltonian show that it exceeds the spacing between real energies of the two-exciton states that gives rise to the transition to the regime of overlapping resonances supplying the system by the new collectivity - the possibility of coherent decay in the annihilation channel. The decay of two-exciton states varies from twice bimolecular decay rate to the much smaller values that is associated with population trapping. We have also considered the corresponding experiment in the framework of our approach, the picture of which appears to be more complex and richer than it was reasoned before.

  13. Exciton Seebeck effect in molecular systems

    SciTech Connect

    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.

  14. Vertically coupled dipolar exciton molecules

    NASA Astrophysics Data System (ADS)

    Cohen, Kobi; Khodas, Maxim; Laikhtman, Boris; Santos, Paulo V.; Rapaport, Ronen

    2016-06-01

    While the interaction potential between two dipoles residing in a single plane is repulsive, in a system of two vertically adjacent layers of dipoles it changes from repulsive interaction in the long range to attractive interaction in the short range. Here we show that for dipolar excitons in semiconductor heterostructures, such a potential may give rise to bound states if two such excitons are excited in two separate layers, leading to the formation of vertically coupled dipolar exciton molecules. Our calculations prove the existence of such bound states and predict their binding energy as a function of the layers separation as well as their thermal distributions. We show that these molecules should be observed in realistic systems such as semiconductor coupled quantum well structures and the more recent van der Waals bound heterostructures. Formation of such molecules can lead to new effects such as a collective dipolar drag between layers and new forms of multiparticle correlations, as well as to the study of dipolar molecular dynamics in a controlled system.

  15. Impurities in Bose-Einstein Condensates: From Polaron to Soliton.

    PubMed

    Shadkhoo, Shahriar; Bruinsma, Robijn

    2015-09-25

    We propose that impurities in a Bose-Einstein condensate which is coupled to a transversely laser-pumped multimode cavity form an experimentally accessible and analytically tractable model system for the study of impurities solvated in correlated liquids and the breakdown of linear-response theory [corrected]. As the strength of the coupling constant between the impurity and the Bose-Einstein condensate is increased, which is possible through Feshbach resonance methods, the impurity passes from a large to a small polaron state, and then to an impurity-soliton state. This last transition marks the breakdown of linear-response theory.

  16. Truncated phase-space approach to polaron response.

    PubMed

    Sels, Dries; Brosens, Fons

    2014-01-01

    A method is presented to obtain the linear response coefficients of a system coupled to a bath. The method is based on a systematic truncation of the Liouville equation for the reduced distribution function. The first-order truncation results are expected to be accurate in the low-temperature and weak-coupling regime. Explicit expressions for the conductivity of the Fröhlich polaron are obtained, and the discrepancy between the Kadanoff and the Feynman-Hellwarth-Iddings-Platzman mobility is elucidated. PMID:24580189

  17. On uniqueness and non-degeneracy of anisotropic polarons

    NASA Astrophysics Data System (ADS)

    Ricaud, Julien

    2016-05-01

    We study the anisotropic Choquard-Pekar equation which describes a polaron in an anisotropic medium. We prove the uniqueness and non-degeneracy of minimizers in a weakly anisotropic medium. In addition, for a wide range of anisotropic media, we derive the symmetry properties of minimizers and prove that the kernel of the associated linearized operator is reduced, apart from three functions coming from the translation invariance, to the kernel on the subspace of functions that are even in each of the three principal directions of the medium.

  18. Distinct exciton dissociation behavior of organolead trihalide perovskite and excitonic semiconductors studied in a same device

    DOE PAGES

    Hu, Miao; Bi, Cheng; Yuan, Yongbo; Xiao, Zhengguo; Dong, Qingfeng; Shao, Yuchuan; Huang, Jinsong

    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.

  19. Superexchange coupling and electron transfer in globular proteins via polaron excitations.

    PubMed

    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.

  20. Cross-polarized excitons in carbon nanotubes.

    PubMed

    Kilina, Svetlana; Tretiak, Sergei; Doorn, Stephen K; Luo, Zhengtang; Papadimitrakopoulos, Fotios; Piryatinski, Andrei; Saxena, Avadh; Bishop, Alan R

    2008-05-13

    Polarization of low-lying excitonic bands in finite-size semiconducting single-walled carbon nanotubes (SWNTs) is studied by using quantum-chemical methodologies. Our calculations elucidate properties of cross-polarized excitons, which lead to the transverse optical absorption of nanotubes and presumably couple to intermediate-frequency modes recently observed in resonance Raman excitation spectroscopy. We identify up to 12 distinct excitonic transitions below the second fundamental band associated with the E(22) van Hove singularity. Calculations for several chiral SWNTs distinguish the optically active "bright" excitonic band polarized parallel to the tube axis and several optically "weak" cross-polarized excitons. The rest are optically (near) forbidden "dark" transitions. An analysis of the transition density matrices related to excitonic bands provides detailed information about delocalization of excitonic wavefunction along the tube. Utilization of the natural helical coordinate system accounting for the tube chirality allows one to disentangle longitudinal and circumferential components. The distribution of the transition density matrix along a tube axis is similar for all excitons. However, four parallel-polarized excitons associated with the E(11) transition are more localized along the circumference of a tube, compared with others related to the E(12) and E(21) cross-polarized transitions. Calculated splitting between optically active parallel- and cross-polarized transitions increases with tube diameter, which compares well with experimental spectroscopic data. PMID:18463293

  1. Cross-polarized excitons in carbon nanotubes

    PubMed Central

    Kilina, Svetlana; Tretiak, Sergei; Doorn, Stephen K.; Luo, Zhengtang; Papadimitrakopoulos, Fotios; Piryatinski, Andrei; Saxena, Avadh; Bishop, Alan R.

    2008-01-01

    Polarization of low-lying excitonic bands in finite-size semiconducting single-walled carbon nanotubes (SWNTs) is studied by using quantum-chemical methodologies. Our calculations elucidate properties of cross-polarized excitons, which lead to the transverse optical absorption of nanotubes and presumably couple to intermediate-frequency modes recently observed in resonance Raman excitation spectroscopy. We identify up to 12 distinct excitonic transitions below the second fundamental band associated with the E22 van Hove singularity. Calculations for several chiral SWNTs distinguish the optically active “bright” excitonic band polarized parallel to the tube axis and several optically “weak” cross-polarized excitons. The rest are optically (near) forbidden “dark” transitions. An analysis of the transition density matrices related to excitonic bands provides detailed information about delocalization of excitonic wavefunction along the tube. Utilization of the natural helical coordinate system accounting for the tube chirality allows one to disentangle longitudinal and circumferential components. The distribution of the transition density matrix along a tube axis is similar for all excitons. However, four parallel-polarized excitons associated with the E11 transition are more localized along the circumference of a tube, compared with others related to the E12 and E21 cross-polarized transitions. Calculated splitting between optically active parallel- and cross-polarized transitions increases with tube diameter, which compares well with experimental spectroscopic data. PMID:18463293

  2. Exciton spin dynamics in GaSe

    SciTech Connect

    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.

  3. Exciton induced photodesorption in rare gas solids

    NASA Astrophysics Data System (ADS)

    Hirayama, Takato; Arakawa, Ichiro

    2006-08-01

    This paper reviews our progress on the desorption induced by electronic transitions (DIET) in rare gas solids by selective excitation of valence excitons. Observation of metastable atoms desorbed by excitonic excitation gives us direct information on the exciton-induced desorption processes in rare gas solids. The validity of three desorption mechanisms, cavity ejection, excimer dissociation, and internal sputtering, is demonstrated by systematic measurements of kinetic energies and angular distributions of desorbed particles. The absolute yield of total and partial desorption was measured, which can lead us to the quantitative understanding of exciton-induced desorption processes.

  4. Exciton Brightening in Monolayer Phosphorene via Dimensionality Modification.

    PubMed

    Xu, Renjing; Yang, Jiong; Myint, Ye Win; Pei, Jiajie; Yan, Han; Wang, Fan; Lu, Yuerui

    2016-05-01

    Exciton brightening in monolayer phosphorene is achieved via the dimensionality modification of excitons from quasi-1D to 0D. The luminescence quantum yield of 0D-like excitons is >33.6 times larger than that of quasi-1D free excitons. 2D phosphorene with quasi-1D free excitons and 0D-like excitons provides a unique platform to investigate the fundamental phenomena in the ideal 2D-1D-0D hybrid system.

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

    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.

  6. Relative ordering between bright and dark excitons in single-walled carbon nanotubes.

    PubMed

    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.

  7. Optical spectroscopy of free excitons in a CuInS{sub 2} chalcopyrite semiconductor compound

    SciTech Connect

    Mudryi, A. V. Ivanyukovich, A. V.; Yakushev, M. V.; Martin, R.; Saad, A.

    2008-01-15

    The spectra of reflectance and luminescence of high-quality CuInS{sub 2} single crystals grown by oriented crystallization are studied at the temperature 4.2 K. In the region of the fundamental absorption edge, the two excitonic resonance reflectance peaks, nondegenerate peak A at the energy {approx}1.5356 eV and doubly degenerate peak BC at the energy {approx}1.5567 eV, and the luminescence signal produced by free and bound excitons are observed. The luminescence lines, A{sub UPB} at {approx}1.5361 eV and A{sub LPB} at {approx}1.5347 eV, with a half-width {approx}1 meV, are attributed to exciton-polariton recombination. From the experimentally observed energy position of the exciton ground state and excited states, the binding energy of free excitons is determined to be {approx}18.5 meV. In studying the photoluminescence in magnetic fields up to 10 T, a diamagnetic shift of the ground state of free excitons A is observed.

  8. Josephson effects in condensates of excitons and exciton polaritons

    NASA Astrophysics Data System (ADS)

    Shelykh, I. A.; Solnyshkov, D. D.; Pavlovic, G.; Malpuech, G.

    2008-07-01

    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.

  9. Josephson effects in condensates of excitons and exciton polaritons

    SciTech Connect

    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.

  10. 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.

  11. Two-dimensional polaronic behavior in the binary oxides m-HfO2 and m-ZrO2.

    PubMed

    McKenna, Keith P; Wolf, Matthew J; Shluger, Alexander L; Lany, Stephan; Zunger, Alex

    2012-03-16

    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 zero-dimensional 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.

  12. Landau levels of the C-exciton in CuInSe{sub 2} studied by magneto-transmission

    SciTech Connect

    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.

  13. Bound exciton and free exciton states in GaSe thin slab

    PubMed Central

    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

  14. DNA-mediated excitonic upconversion FRET switching

    SciTech Connect

    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.

  15. DNA-mediated excitonic upconversion FRET switching

    DOE PAGES

    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 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

  16. Exciton luminescence of 8-azasteroid microcrystals

    NASA Astrophysics Data System (ADS)

    Akhrem, A. A.; Borisevich, N. A.; Gulyakevich, O. V.; Knyukshto, V. N.; Mikhal'Chuk, A. L.; Tikhomirov, S. A.; Tolstorozhev, G. B.

    1999-05-01

    Luminescence of microcrystals of 2,3-methoxy-8-azagon-1,3,5(10),13-tetraene-12,17-dion of the class of molecules of biologically active steroids is detected at room temperature (293 K). It represents fast fluorescence of free and self-localized excitons and prolonged phosphorescence of triplet excitons.

  17. DNA-mediated excitonic upconversion FRET switching

    NASA Astrophysics Data System (ADS)

    Kellis, Donald L.; Rehn, Sarah M.; Cannon, Brittany L.; Davis, Paul H.; Graugnard, Elton; Lee, Jeunghoon; Yurke, Bernard; Knowlton, William B.

    2015-11-01

    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 upconversion via upconversion nanoparticles (UCNPs), although currently inefficient, serves as an energy ratchet to boost the exciton energy. Although FRET-based upconversion has been demonstrated, it suffers from low FRET efficiency and lacks the ability to modulate the FRET. We have engineered an upconversion FRET-based switch by combining lanthanide-doped UCNPs and fluorophores that demonstrates excitonic energy upconversion 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 upconversion in nanophotonic applications including artificial light harvesting, excitonic circuits, photovoltaics, nanomedicine, and optoelectronics.

  18. Subnanosecond control of excitons in coupled quantum well nanostructures: Photonic storage and Exciton Conveyer devices

    NASA Astrophysics Data System (ADS)

    Winbow, Alexander Graham

    Indirect excitons in GaAs coupled quantum well nanostructures are a versatile system for fundamental study of cold neutral bosonic gases and demonstration of novel optoelectronic devices based on excitons --- a bound electron--hole pair --- rather than electrons. Indirect exciton lifetimes range from nanoseconds to microseconds and cool rapidly after photoexcitation to the lattice temperature. Lithographically-patterned electrodes enable design of potential energy landscapes, and both energy and lifetime can be controlled in situ, rapidly, on timescales much shorter than the exciton lifetime. Such intrinsically optoelectronic devices can operate at speeds relevant to optical networks, and later be fabricated in other semiconductors for higher-temperature operation. Two different kinds of devices are demonstrated: Photon storage --- an optical memory --- with 250 ps rise time of the readout optical signal and storage time reaching microseconds was implemented with indirect excitons in CQW. The storage and release of photons was controlled by the gate voltage pulse, and the transient processes in the CQW studied by measuring the kinetics of the exciton emission spectra. This control of excitons on timescales much shorter than the exciton lifetime demonstrates the feasibility of studying excitons in in situ controlled electrostatic traps. The Exciton Conveyer is a laterally moving electrostatic lattice potential for actively transporting excitons. Generated by laterally modulated electrodes, the potential velocity and depth are controlled in situ by frequency and voltage. We observed exciton transport characterized by average exciton cloud spatial extension over several tens of microns, and observed dynamical localization--delocalization transitions for the excitons in the conveyer: In the localization regime of deeper potentials and moderate exciton density, excitons are moved by the conveyer; in the delocalized regime of shallower lattice potential or high exciton

  19. Charge carriers and small-polaron migration as the origin of intrinsic dielectric anomalies in multiferroic TbMnO3 polycrystals.

    PubMed

    Silveira, L G D; Dias, G S; Cótica, L F; Eiras, J A; Garcia, D; Sampaio, J A; Yokaichiya, F; Santos, I A

    2013-11-27

    Temperature-dependent and frequency-dependent dielectric investigations have been performed in TbMnO3 polycrystals sintered in either oxidative or reductive atmospheres. The results revealed the occurrence of two dielectric anomalies above 100 K, which are caused by the thermal activation of charge carriers and their motion in grain cores and grain boundaries. The temperature dependence of the bulk dc conductivity was also analysed and indicates that charge carriers move between inequivalent sites according to a variable-range-hopping mechanism. Also, a strong correlation between dielectric properties and crystalline structure was observed. Furthermore, a low-temperature dielectric relaxation, commonly reported in rare-earth manganite crystals, was observed in both samples. This relaxation follows the empirical Cole-Cole model and was attributed to small-polaron tunnelling. Polaron motion was observed to be affected by the magnetic transitions, structural properties and intrinsic anisotropies in TbMnO3. It is also worth mentioning that the dielectric anomaly due to motion of charge carriers in grain boundaries is the only one of extrinsic origin, while the anomalies related to carrier motion in grain cores and small-polaron tunnelling are intrinsic to TbMnO3.

  20. 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.

  1. Excitonic energy transfer in light-harvesting complexes in purple bacteria.

    PubMed

    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.

  2. Excitonic energy transfer in light-harvesting complexes in purple bacteria

    SciTech Connect

    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.

  3. Influence of lithium vacancies on the polaronic transport in olivine phosphate structure

    NASA Astrophysics Data System (ADS)

    Murugavel, Sevi; Sharma, Monika; Shahid, Raza

    2016-01-01

    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 LiFePO4 (LFP) and delithiated heterosite FePO4 (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.

  4. Recombination lifetime of free polarons in polymer/fullerene bulk heterojunction solar cells

    NASA Astrophysics Data System (ADS)

    Li, Kejia; Li, Lijun; Campbell, Joe C.

    2012-02-01

    The recombination lifetime of free polarons was measured using three different methods: electrical field-dependent photoresponse, transient photoconductivity, and forward-to-zero bias transient-current response. The average free polaron recombination lifetime is estimated to be a few microseconds for poly (3-hexylthiophene) (P3HT) and [6,6]-phenyl C61-butyric acid methyl ester (PCBM) solar cells. The competition between sweep-out by the internal field and the loss of photogenerated carriers by recombination is analyzed. The short-circuit free polaron collection efficiency for P3HT:PCBM bulk heterojunction material was determined to be in the range of 80% to 90%.

  5. Atomistic model for excitons: Capturing Strongly Bound Excitons in Monolayer Transition-Metal Dichalcogenides

    NASA Astrophysics Data System (ADS)

    Tseng, Frank; Simsek, Ergun; Gunlycke, Daniel

    2015-03-01

    Monolayer transition-metal dichalcogenides form a direct bandgap predicted in the visible regime making them attractive host materials for various electronic and optoelectronic applications. Due to a weak dielectric screening in these materials, strongly bound electron-hole pairs or excitons have binding energies up to at least several hundred meV's. While the conventional wisdom is to think of excitons as hydrogen-like quasi-particles, we show that the hydrogen model breaks down for these experimentally observed strongly bound, room-temperature excitons. To capture these non-hydrogen-like photo-excitations, we introduce an atomistic model for excitons that predicts both bright excitons and dark excitons, and their broken degeneracy in these two-dimensional materials. For strongly bound exciton states, the lattice potential significantly distorts the envelope wave functions, which affects predicted exciton peak energies. The combination of large binding energies and non-degeneracy of exciton states in monolayer transition metal dichalogendies may furthermore be exploited in room temperature applications where prolonged exciton lifetimes are necessary. This work has been funded by the Office of Naval Research (ONR), directly and through the Naval Research Laboratory (NRL). F.T and E.S acknowledge support from NRL through the NRC Research Associateship Program and ONR Summer Faculty Program, respectively.

  6. Magnetic Studies of Photovoltaic Processes in Organic Solar Cells

    SciTech Connect

    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.

  7. Polaron transport in TiO{sub 2} thin films

    SciTech Connect

    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

  8. Dispersed Polaron Simulations of Electron Transfer in Photosynthetic Reaction Centers

    NASA Astrophysics Data System (ADS)

    Warshel, A.; Chu, Z. T.; Parson, W. W.

    1989-10-01

    A microscopic method for simulating quantum mechanical, nuclear tunneling effects in biological electron transfer reactions is presented and applied to several electron transfer steps in photosynthetic bacterial reaction centers. In this ``dispersed polaron'' method the fluctuations of the protein and the electron carriers are projected as effective normal modes onto an appropriate reaction coordinate and used to evaluate the quantum mechanical rate constant. The simulations, based on the crystallographic structure of the reaction center from Rhodopseudomonas viridis, focus on electron transfer from a bacteriopheophytin to a quinone and the subsequent back-reaction. The rates of both of these reactions are almost independent of temperature or even increase with decreasing temperature. The simulations reproduce this unusual temperature dependence in a qualitative way, without the use of adjustable parameters for the protein's Franck-Condon factors. The observed dependence of the back-reaction on the free energy of the reaction also is reproduced, including the special behavior in the ``inverted region.''

  9. Magnetic field effect spectroscopy of C60-based films and devices

    NASA Astrophysics Data System (ADS)

    Gautam, Bhoj R.; Nguyen, Tho D.; Ehrenfreund, Eitan; Vardeny, Z. Valy

    2013-04-01

    We performed spectroscopy of the magnetic field effect (MFE) including magneto-photoinduced absorption (MPA) and magneto-photoluminescence (MPL) at steady state conditions in annealed and pristine fullerene C60 thin films, as well as magneto-conductance (MC) in organic diodes based on C60 interlayer. The hyperfine interaction has been shown to be the primary spin mixing mechanism for the MFE in the organics. In this respect, C60 is a unique material because 98.9% of the carbon atoms are 12C isotope, having spinless nucleus and thus lack hyperfine interaction. In spite of this, we obtained substantial MPA (up to ˜15%) and significant MC and MPL in C60 films and devices, and thus mechanisms other than the hyperfine interaction are responsible for the MFE in this material. Specifically, we found that the MFE(B) response is composed of narrow (˜10 mT) and broad (>100 mT) components. The narrow MFE(B) component is due to spin-dependent triplet exciton recombination in C60, which dominates the MPA(B) response at low pump intensities in films, or the MC response at small current densities in devices. In contrast, the broad MFE(B) component dominates the MPA(B) response at high pump intensities (or large current densities for MC(B)) and is attributed to spin mixing in the polaron pairs spin manifold due to g-factor mismatch between the electron- and hole-polarons in C60. Our results show that the organic MFE has a much broader scope than believed before.

  10. 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.

  11. Polaronic conduction and Anderson localization in reduced strontium barium niobate

    NASA Astrophysics Data System (ADS)

    Dandeneau, Christopher S.; Yang, YiHsun; Olmstead, Marjorie A.; Bordia, Rajendra K.; Ohuchi, Fumio S.

    2015-12-01

    Electron transport mechanisms in reduced Sr0.5Ba0.5Nb2O6 (SBN50) are investigated from ˜100 to 955 K through an analysis of the electrical conductivity (σ) and the Seebeck coefficient (S) with respect to temperature (T). Notably, experimental evidence is presented that supports a scenario of Anderson localization below 600 K and carrier excitation across a mobility edge at higher temperature. As a relaxor ferroelectric, stoichiometric SBN has intrinsic disorder associated with both the distribution of Sr/Ba vacancies and the formation of polarized nanoregions. The removal of oxygen through reduction generates conduction electrons in SBN. At the lowest temperatures measured (100-155 K), the electrical conductivity exhibits a temperature dependence characteristic of variable range hopping, followed by a transition to small polaron hopping at intermediate temperatures (250-545 K). In both the variable range and small polaron hopping regimes, a semiconductor-like temperature dependence of the electrical conductivity (dσ/dT > 0) was observed. However, above 615 K, dσ/dT decreases dramatically and eventually becomes metal-like (dσ/dT < 0). Concomitantly, the Seebeck coefficient exhibits a linear dependence on lnT from 615 to 955 K with the same slope (˜104 μ V/K) for both polycrystalline SBN50 and single crystalline SBN61 (both reduced), indicating a similar, constant density of states near the Fermi level for both compositions. The application of Seebeck coefficient theory to this inherently disordered material reveals that the excitation of carriers across a mobility edge is likely responsible for the change in dσ/dT at high temperature. Such findings may have a significant impact in the field of conductive ferroelectrics.

  12. Exciton-Polariton Dynamics in Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Bondarev, Igor

    2007-03-01

    This work addresses theoretically the nonlinear response of phonon-coupled excitons[1] in carbon nanotubes to an external electromagnetic field. The photon Green's function approach developed recently to quantize the electromagnetic field in the presence of quasi-1D absorbing bodies[2],[3] is being used to study the dynamics of phonon-coupled excitonic states interacting with the surface photonic modes excited by the external electromagnetic field in semiconductor carbon nanotubes. The formation of the new elementary excitations, exciton-polaritons, representing the eigen states of the full photon-matter Hamiltonian has been studied for small-diameter nanotubes under strong exciton-photon coupling. Time-resolved simulations have been performed of the coherent exciton- polariton dynamics with the exciton-phonon interactions taken into account. The criteria for the coherent control of the excitonic states population in optically excited carbon nanotubes have been formulated. [1]F.Plentz et al, Phys. Rev. Lett. 95, 247401 (2005). [2]I.V.Bondarev and Ph.Lambin, Phys. Rev. B 72, 035451 (2005). [3]I.V.Bondarev and Ph.Lambin, in: Trends in Nanotubes Reasearch (NovaScience, New York, 2006), p.139.

  13. Dimensional magnetoplasma resonance detected by free-exciton photoluminescence in modulation-doped GaAs/AlxGa1-xAs heterojunctions

    NASA Astrophysics Data System (ADS)

    Ashkinadze, B. M.; Linder, E.; Umansky, V.

    2000-10-01

    We studied the effect of microwave (mw) irradiation on the low-temperature photoluminescence (PL) of high-quality, modulation-doped, wide GaAs/AlxGa1-xAs heterojunctions (HJ's) containing a two-dimensional electron gas (2DEG), in the density range of (0.9-4)×1011 cm-2. The PL arises from excitons that recombine radiatively in the GaAs buffer layer, far from the 2DEG which is confined close to the GaAs/AlxGa1-xAs interface. We observe that the exciton PL is affected by a mw heating of the 2DEG: the mw-induced PL intensity change increases with increasing 2DEG density as well as under a perpendicular magnetic field that corresponds to the 2DEG dimensional magnetoplasma resonance (DMPR) condition. Moreover, the exciton PL intensity shows a bistability at magnetic field strengths that are close to those observed in the DMPR mw absorption. The mw-induced PL modulation effects are interpreted as being due to the interaction of the excitons with low-energy, ballistically propagating acoustic phonons that are emitted by the mw-heated 2DEG. The exciton PL quenching is associated with an exciton drag by the phonon flux towards the opposite HJ interface where the excitons recombine nonradiatively. The rate of phonon emission is determined by the 2DEG state, and thus the exciton PL responds to the changes of the 2DEG parameters.

  14. Illumination induced metastable polaron-supporting phase in poly p-phenylene- vinylene films

    NASA Astrophysics Data System (ADS)

    Ehrenfreund, E.; Gershman, E.; Eichen, Y.; Drori, T.; Sheng, C. X.; Vardeny, Z. V.

    2007-03-01

    We found a new illumination induced metastable polaron-supporting phase in pristine films of a soluble derivative of poly-p-phenylene vinylene (MEH-PPV). In the pristine, un-illuminated MEH-PPV phase A, the polymer films do not show any long-lived photogenerated polarons. Prolonged UV illumination, however, was found to induce a reversible, metastable phase B, characterized by its ability to support the existence of abundant long-lived photogenerated polarons. In the dark, films of phase B revert back to the original phase A within about thirty minutes at room temperature. Relying on the well-established ubiquitous reversible photoinduced cyclization of diarylethenes into dihyrophenanthrene derivatives, we propose a reversible mechanism in which UV illumination creates metastable deep defects that substantially increase the photogenerated polaron lifetime.

  15. Illumination-induced metastable polaron-supporting state in poly( p -phenylene vinylene) films

    NASA Astrophysics Data System (ADS)

    Drori, T.; Gershman, E.; Sheng, C. X.; Eichen, Y.; Vardeny, Z. V.; Ehrenfreund, E.

    2007-07-01

    We found an illumination-induced metastable polaron-supporting state in films of a soluble derivative of poly- p -phenylene vinylene (MEH-PPV). Pristine, nonilluminated MEH-PPV polymer films do not show long-lived photogenerated polarons. Prolonged UV illumination, however, is found to induce a reversible, metastable state characterized by its ability to support abundant long-lived photogenerated polarons. In the dark, the illumination-induced metastable state reverts back to the state of the original MEH-PPV within about 30min at room temperature. Relying on the well-established ubiquitous reversible photoinduced cyclization of diarylethenes into dihyrophenanthrene derivatives, we propose a reversible mechanism in which UV illumination transforms cis native defects in the polymer chains into metastable deep traps that substantially increase the photogenerated polaron lifetime in the film.

  16. Exciton storage in type-II quantum dots using the optical Aharonov-Bohm effect

    SciTech Connect

    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.

  17. Multiple Exciton Generation Solar Cells

    SciTech Connect

    Luther, J. M.; Semonin, O. E.; Beard, M. C.; Gao, J.; Nozik, A. J.

    2012-01-01

    Heat loss is the major factor limiting traditional single junction solar cells to a theoretical efficiency of 32%. Multiple Exciton Generation (MEG) enables efficient use of the solar spectrum yielding a theoretical power conversion efficiency of 44% in solar cells under 1-sun conditions. Quantum-confined semiconductors have demonstrated the ability to generate multiple carriers but present-day materials deliver efficiencies far below the SQ limit of 32%. Semiconductor quantum dots of PbSe and PbS provide an active testbed for developing high-efficiency, inexpensive solar cells benefitting from quantum confinement effects. Here, we will present recent work of solar cells employing MEG to yield external quantum efficiencies exceeding 100%.

  18. Laser Asisted Scattering of an Optical Polaron in Presence of an Impurity Center

    NASA Astrophysics Data System (ADS)

    Mukhopadhyay, S.; Sinha, C.

    2012-11-01

    Momentum transfer cross-sections are studied for polarons inside a polar medium in presence of a coulomb impurity center as well as an external linerly polarised,homogeneous annd monochromatic laser field. The strongly bound polaron is found to be reluctant to contribute to the conductivity which is justified physically. The present study may find application in development of electronic devices using polar materials like organic semiconductors.

  19. [Long-range electron transfer in globular proteins by polaron excitation].

    PubMed

    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.

  20. 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.

  1. External quantum efficiency above 100% in a singlet-exciton-fission-based organic photovoltaic cell.

    PubMed

    Congreve, Daniel N; Lee, Jiye; Thompson, Nicholas J; Hontz, Eric; Yost, Shane R; Reusswig, Philip D; Bahlke, Matthias E; Reineke, Sebastian; Van Voorhis, Troy; Baldo, Marc A

    2013-04-19

    Singlet exciton fission transforms a molecular singlet excited state into two triplet states, each with half the energy of the original singlet. In solar cells, it could potentially double the photocurrent from high-energy photons. We demonstrate organic solar cells that exploit singlet exciton fission in pentacene to generate more than one electron per incident photon in a portion of the visible spectrum. Using a fullerene acceptor, a poly(3-hexylthiophene) exciton confinement layer, and a conventional optical trapping scheme, we show a peak external quantum efficiency of (109 ± 1)% at wavelength λ = 670 nanometers for a 15-nanometer-thick pentacene film. The corresponding internal quantum efficiency is (160 ± 10)%. Analysis of the magnetic field effect on photocurrent suggests that the triplet yield approaches 200% for pentacene films thicker than 5 nanometers. PMID:23599489

  2. Exciton Hierarchies in Gapped Carbon Nanotubes

    SciTech Connect

    Konik, R.M.

    2011-04-01

    We present evidence that the strong electron-electron (e-e) interactions in gapped carbon nanotubes lead to finite hierarchies of excitons within a given nanotube subband. We study these hierarchies by employing a field theoretic reduction of the gapped carbon nanotube permitting e-e interactions to be treated exactly. We analyze this reduction by employing a Wilsonian-like numerical renormalization group. We are so able to determine the gap ratios of the one-photon excitons as a function of the effective strength of interactions. We also determine within the same subband the gaps of the two-photon excitons, the single particle gaps, as well as a subset of the dark excitons. The strong e-e interactions in addition lead to strongly renormalized dispersion relations where the consequences of spin-charge separation can be readily observed.

  3. Exciton hierarchies in gapped carbon nanotubes.

    PubMed

    Konik, Robert M

    2011-04-01

    We present evidence that the strong electron-electron (e-e) interactions in gapped carbon nanotubes lead to finite hierarchies of excitons within a given nanotube subband. We study these hierarchies by employing a field theoretic reduction of the gapped carbon nanotube permitting e-e interactions to be treated exactly. We analyze this reduction by employing a Wilsonian-like numerical renormalization group. We are so able to determine the gap ratios of the one-photon excitons as a function of the effective strength of interactions. We also determine within the same subband the gaps of the two-photon excitons, the single particle gaps, as well as a subset of the dark excitons. The strong e-e interactions in addition lead to strongly renormalized dispersion relations where the consequences of spin-charge separation can be readily observed.

  4. Cavity-Enhanced Transport of Excitons

    NASA Astrophysics Data System (ADS)

    Schachenmayer, Johannes; Genes, Claudiu; Tignone, Edoardo; Pupillo, Guido

    2015-05-01

    We show that exciton-type transport in certain materials can be dramatically modified by their inclusion in an optical cavity: the modification of the electromagnetic vacuum mode structure introduced by the cavity leads to transport via delocalized polariton modes rather than through tunneling processes in the material itself. This can help overcome exponential suppression of transmission properties as a function of the system size in the case of disorder and other imperfections. We exemplify massive improvement of transmission for excitonic wave packets through a cavity, as well as enhancement of steady-state exciton currents under incoherent pumping. These results may have implications for experiments of exciton transport in disordered organic materials. We propose that the basic phenomena can be observed in quantum simulators made of Rydberg atoms, cold molecules in optical lattices, as well as in experiments with trapped ions.

  5. 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.

  6. 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.

  7. Hybrid interlayer excitons with tunable dispersion relation

    NASA Astrophysics Data System (ADS)

    Skinner, Brian

    When two semiconducting materials are layered on top of each other, interlayer excitons can be formed by the Coulomb attraction of an electron in one layer to a hole in the opposite layer. The resulting exciton is a composite boson with a dispersion relation that is a hybrid between the dispersion relations of the electron and the hole separately. In this talk I show how such hybridization is particularly interesting when one layer has a ``Mexican hat''-shaped dispersion relation and the other has a conventional parabolic dispersion. In this case the interlayer exciton can have a range of qualitatively different dispersion relations, which can be continuously altered by an external field. This tunability in principle allows one to continuously tune a collection of interlayer excitons between different quantum many-body phases, including Bose-Einstein condensate, Wigner crystal, and fermion-like ``moat band'' phases.

  8. 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.

  9. Excitons and spin-dependent optical effects in semiconductor quantum dots

    NASA Astrophysics Data System (ADS)

    Govorov, Alexander; Warburton, Richard; Karrai, Khaled

    2004-04-01

    We discuss the possibility of entangling a localized exciton in a quantum dot with delocalized electrons in adjacent continuum states. We present two mechanisms by which this can occur, both involving excitons in InAs self-assembled quantum dots. The first mechanism involves a tunnel hybridization between weakly-confined electron states in the quantum dot and delocalized states in the continuum [1]. By describing the hybridization with the Anderson Hamiltonian we discover theoretically the existence of novel exciton states which can be called Kondo excitons [1]. We predict several optical manifestations of Kondo excitons. The second mechanism corresponds to an intra-dot Auger-like process [2,3]. Experiments in a magnetic field strongly support the picture of Auger-like processes [2]. [1] A.O. Govorov, R. J. Warburton, and K. Karrai, Phys. Rev. B RC, 67, 241307 (2003). [2] R.J. Warburton, B. Urbaszek, E.J. McGhee, C. Schulhauser, A. Hogele, K. Karrai, A.O.Govorov, J.M. Garcia, B.D.Gerardot, and P.M. Petroff, Nature 427, 135 (2004). [3] A. O. Govorov, K. Karrai, R. J. Warburton, and A. V. Kalameitsev, Physica E, 295 (2004).

  10. 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.

  11. 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

  12. Anisotropic exciton Stark shift in black phosphorus

    NASA Astrophysics Data System (ADS)

    Chaves, A.; Low, Tony; Avouris, P.; ćakır, D.; Peeters, F. M.

    2015-04-01

    We calculate the excitonic spectrum of few-layer black phosphorus by direct diagonalization of the effective mass Hamiltonian in the presence of an applied in-plane electric field. The strong attractive interaction between electrons and holes in this system allows one to investigate the Stark effect up to very high ionizing fields, including also the excited states. Our results show that the band anisotropy in black phosphorus becomes evident in the direction-dependent field-induced polarizability of the exciton.

  13. Theory of Orbital Susceptibility on Excitonic Insulator

    NASA Astrophysics Data System (ADS)

    Matsuura, Hiroyasu; Ogata, Masao

    2016-09-01

    We study the temperature dependence of the orbital susceptibility of an excitonic insulator on the basis of a two-band model. It is shown that a drastic change (an anomalous enhancement) in susceptibility as a function of temperature occurs owing to the occurrence of additional orbital susceptibility due to the excitonic gap. We calculate explicitly the temperature dependence of orbital susceptibility for a model of Ta2NiSe5, and show that the result is consistent with experimental results.

  14. Exciton transport by surface acoustic waves

    NASA Astrophysics Data System (ADS)

    Rudolph, J.; Hey, R.; Santos, P. V.

    2007-05-01

    Long-range acoustic transport of excitons in GaAs quantum wells (QWs) is demonstrated. The mobile strain field of a surface acoustic wave creates a dynamic lateral type I modulation of the conduction and valence bands in a double-quantum-well (DQW) structure. This mobile potential modulation transports long-living indirect excitons in the DQW over several hundreds of μm.

  15. 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.

  16. Exciton quasicondensation in one-dimensional systems

    NASA Astrophysics Data System (ADS)

    Werman, Yochai; Berg, Erez

    2015-06-01

    Two Luttinger liquids, with an equal density and opposite sign of charge carriers, may exhibit enhanced excitonic correlations. We term such a system an exciton quasicondensate, with a possible realization being two parallel oppositely doped quantum wires, coupled by repulsive Coulomb interactions. We show that this quasiexciton condensate can be stabilized in an extended range of parameters, in both spinless and spinful systems. We calculate the interwire tunneling current-voltage characteristic, and find that a negative differential conductance is a signature of excitonic correlations. For spinful electrons, the excitonic regime is shown to be distinct from the usual quasi-long-range ordered Wigner crystal phase characterized by power-law density wave correlations. The two phases can be clearly distinguished through their interwire tunneling current-voltage characteristics. In the quasiexciton condensate regime the tunneling conductivity diverges at low temperatures and voltages, whereas in the Wigner crystal it is strongly suppressed. Both the Wigner crystal and the excitonic regime are characterized by a divergent Coulomb drag at low temperature. Finally, metallic carbon nanotubes are considered as a special case of such a one-dimensional setup, and it is shown that exciton condensation is favorable due to the additional valley degree of freedom.

  17. Surface Exciton-Plasmons in Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Bondarev, Igor; Tatur, Kevin; Woods, Lilia

    2008-03-01

    We study theoretically the interactions of excitonic states with surface electromagnetic modes of a single-walled carbon nanotube. We use our previously developed Green's function formalism to quantize an electromagnetic field in the presence of quasi-1D absorbing bodies [1]. We show that these interactions result in the exciton-plasmon coupling that is significant in its strength due to the presence of weakly-dispersive low-energy (˜0.5-2eV) interband surface plasmon modes [2] and large exciton excitation energies ˜1eV in small-diameter nanotubes [3]. We estimate the exciton-plasmon Rabi splitting to be ˜0.01-0.1eV which is close to that observed in organic semiconductors [4] and much larger than that reported for hybrid semiconductor-metal nanoparticle molecules [5]. We calculate the exciton absorption lineshape and demonstrate a clear line splitting effect as the exciton energy is tuned to the closest interband surface plasmon resonance. [1] I.V.Bondarev and Ph.Lambin, Phys. Rev. B72, 035451 (2005). [2] T.Pichler, et al., Phys. Rev. Lett. 80, 4729 (1998). [3] D.Spataru, et al., Phys. Rev. Lett. 95, 247402 (2005). [4] J.Belessa, et al., Phys. Rev. Lett. 93, 036404 (2004). [5] W.Zhang, A.O.Govorov, G.W.Bryant, Phys. Rev. Lett. 97, 146804 (2006).

  18. Magnetic resonance in films and photodiodes based on poly-(phenyl-phenylene-vinylene)

    NASA Astrophysics Data System (ADS)

    Dyakonov, V.; Rösler, G.; Schwoerer, M.; Blumstengel, S.; Lüders, K.

    1996-02-01

    Films of poly-(2-phenyl-1,4-phenylene-vinylene) (PPPV) and photodiodes with PPPV as an active layer were studied by optically (ODMR) and electrically (EDMR) detected electron-spin resonance (ESR). Two different signals were observed in ODMR: enhancement of the photoluminescence (PL) at g=2.01 due to recombination of the photogenerated polarons (s=1/2), and a half-field enhancement signal, attributed to the fusion of triplet excitons. Both processes lead to the formation of singlet excitons. The spectral dependence of the s=1/2 signal follows the low energy part of the PL spectrum, indicating that delayed recombination of distant polarons is influenced by ESR, whereas the cw PL contains both prompt and delayed contributions. The linewidth and the intensity of the ODMR signal depend on the PL excitation intensity. Both effects are due to a decrease of the recombination lifetime of the polaron pairs at higher intensities. The relative decrease of the short-circuit photocurrent ISC through a PPPV photodiode by ESR saturation is due to recombination of nonthermalized, nongeminate excess charge polarons in the active layer of the device. This effect is at least two orders of magnitude stronger than the enhancement of total PL at the same temperature. This feature is found to be common for conjugated polymers investigated so far, and reflects the fact that the total photogenerated ISC is spin dependent, whereas ODMR selects only the nongeminate portion of recombining species in the sample.

  19. Thermodynamics of the polaron master equation at finite bias

    SciTech Connect

    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.

  20. Excitons in the optical properties of nanotubes

    NASA Astrophysics Data System (ADS)

    Spataru, Catalin

    2006-03-01

    We present ab initio calculation of self-energy and electron-hole interaction (excitonic) effects on the optical spectra of single-walled carbon and BN nanotubes. We employed a many-electron Green's function approach that determines both the quasiparticle and optical excitations from first principles. We found important many-electron effects that explain many of the puzzling experimental findings in the optical spectrum of these quasi-one dimensional systems, and the calculated spectra are in excellent quantitative agreement with measurements. In carbon nanotubes, excitons can bind by as much as one eV in semiconducting nanotubes^a). We discovered that bound excitons also exist in metallic carbon nanotubes with binding energy of many tens of meVs^a). Excitonic effects are shown to be even more inportant in BN nanotubes than in carbon nanotubes. Unlike the carbon nanotubes, theory predicts that excitons in some BN nanotubes are comprised of coherent superposition of transitions from several different subband pairs^b). We have also calculated the radiative lifetime of excitons in semiconducting carbon nanotubes. Assuming a thermal occupation of bright and dark exciton bands, we find an effective radiative lifetime of the order of 10 ns at room temperature, in good accord with recent experiments^c). a) C.D. Spataru, S. Ismail-Beigi, L.X. Benedict and S.G. Louie, Phys. Rev. Lett. 92, 077402 (2004). b) C.-H. Park, C.D. Spataru and S.G. Louie, to be published. c) C.D. Spataru, S. Ismail-Beigi, R.B. Capaz and S.G. Louie, in press Phys. Rev. Lett.

  1. 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

  2. Tunable Polarons of Slow-Light Polaritons in a Two-Dimensional Bose-Einstein Condensate.

    PubMed

    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. PMID:26894712

  3. 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.

  4. Tunable Polarons of Slow-Light Polaritons in a Two-Dimensional Bose-Einstein Condensate.

    PubMed

    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.

  5. 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.

  6. Plasmon-Exciton Coupling Using DNA Templates.

    PubMed

    Roller, Eva-Maria; Argyropoulos, Christos; Högele, Alexander; Liedl, Tim; Pilo-Pais, Mauricio

    2016-09-14

    Coherent energy exchange between plasmons and excitons is a phenomenon that arises in the strong coupling regime resulting in distinct hybrid states. The DNA-origami technique provides an ideal framework to custom-tune plasmon-exciton nanostructures. By employing this well controlled self-assembly process, we realized hybrid states by precisely positioning metallic nanoparticles in a defined spatial arrangement with fixed nanometer-sized interparticle spacing. Varying the nanoparticle diameter between 30 nm and 60 nm while keeping their separation distance constant allowed us to precisely adjust the plasmon resonance of the structure to accurately match the energy frequency of a J-aggregate exciton. With this system we obtained strong plasmon-exciton coupling and studied far-field scattering at the single-structure level. The individual structures displayed normal mode splitting up to 170 meV. The plasmon tunability and the strong field confinement attained with nanodimers on DNA-origami renders an ideal tool to bottom-up assembly plasmon-exciton systems operating at room temperature. PMID:27531635

  7. Plasmon-Exciton Coupling Using DNA Templates.

    PubMed

    Roller, Eva-Maria; Argyropoulos, Christos; Högele, Alexander; Liedl, Tim; Pilo-Pais, Mauricio

    2016-09-14

    Coherent energy exchange between plasmons and excitons is a phenomenon that arises in the strong coupling regime resulting in distinct hybrid states. The DNA-origami technique provides an ideal framework to custom-tune plasmon-exciton nanostructures. By employing this well controlled self-assembly process, we realized hybrid states by precisely positioning metallic nanoparticles in a defined spatial arrangement with fixed nanometer-sized interparticle spacing. Varying the nanoparticle diameter between 30 nm and 60 nm while keeping their separation distance constant allowed us to precisely adjust the plasmon resonance of the structure to accurately match the energy frequency of a J-aggregate exciton. With this system we obtained strong plasmon-exciton coupling and studied far-field scattering at the single-structure level. The individual structures displayed normal mode splitting up to 170 meV. The plasmon tunability and the strong field confinement attained with nanodimers on DNA-origami renders an ideal tool to bottom-up assembly plasmon-exciton systems operating at room temperature.

  8. Photoinduced gap closure in an excitonic insulator

    NASA Astrophysics Data System (ADS)

    Golež, Denis; Werner, Philipp; Eckstein, Martin

    2016-07-01

    We study the dynamical phase transition out of an excitonic insulator phase after photoexcitation using a time-dependent extension of the self-consistent GW method. We connect the evolution of the photoemission spectra to the dynamics of the excitonic order parameter and identify two dynamical phase transition points marked by a slowdown in the relaxation: one critical point is connected with the trapping in a nonthermal state with reduced exciton density and the second corresponds to the thermal phase transition. The transfer of kinetic energy from the photoexcited carriers to the exciton condensate is shown to be the main mechanism for the gap melting. We analyze the low energy dynamics of screening, which strongly depends on the presence of the excitonic gap, and argue that it is difficult to interpret the static component of the screened interaction as the effective interaction of some low energy model. Instead we propose a phenomenological measure for the effective interaction which indicates that screening has minor effects on the low energy dynamics.

  9. Probing ultrafast excitation energy transfer of the chlorosome with exciton-phonon variational dynamics.

    PubMed

    Somoza Márquez, Alejandro; Chen, Lipeng; Sun, Kewei; Zhao, Yang

    2016-07-27

    The chlorosome antenna complex is a fascinating structure which due to its immense scale, accurate simulation of excitation energy transfer (EET) dynamics supposes a genuine computational challenge. Resonant vibronic modes have been recently identified in 2D spectra of the chlorosome which motivates our present endeavour of modelling electronic and vibrational degrees of freedom on an equal footing. Following the Dirac-Frenkel time-dependent variational principle, we exploit a general theory of polaron dynamics in two-dimensional lattices based on the Holstein molecular crystal model and investigate a single rod model of pigment aggregates. Unlike reduced formalisms, explicit integration of the degrees of freedom of both the system and the bath requires extensive computational resources. We exploit the architecture of graphic processor units (GPUs) by implementing our simulations on this platform. The simulation of dynamic properties of hundreds or even thousands of pigments is thus achievable in just a few hours. The potential investigation and design of natural or engineered two-dimensional pigment networks can thus be accommodated. Due to the lack of consensus regarding the precise arrangement of chromophores in the chlorosome, helicity and dimerization are investigated independently, extracting their contributions to both optical and EET properties. The presence of dimerization is found to slow down the delocalization process. Exciton delocalization is completed in 100 fs in a single rod aggregate whose dimensions (20 nm) fairly exceed the estimated extent of a coherent domain. Ultrafast energy relaxation in the exciton manifold occurs in 50 fs and the duration of super-diffusive transport is found to last for about 80 fs. PMID:26792106

  10. Optical and spin properties of localized and free excitons in GaBi x As1-x /GaAs multiple quantum wells

    NASA Astrophysics Data System (ADS)

    Balanta, M. A. G.; Kopaczek, J.; Orsi Gordo, V.; Santos, B. H. B.; Rodrigues, A. D.; Galeti, H. V. A.; Richards, R. D.; Bastiman, F.; David, J. P. R.; Kudrawiec, R.; Galvão Gobato, Y.

    2016-09-01

    Raman spectroscopy and magneto-photoluminescence measurements under high magnetic fields were used to investigate the optical and spin properties of GaBiAs/GaAs multiple quantum wells (MQWs). An anomalous negative diamagnetic energy shift was observed at higher temperatures and higher laser intensities, which was associated to a sign inversion of hole effective mass in these structures. In addition, an enhancement of the polarization degree with decreasing of laser intensity was observed (experimental condition where the emission is dominated by localized excitons). This effect was explained by changes of spin relaxation and exciton recombination times due to exciton localization by disorder.

  11. Optical and spin properties of localized and free excitons in GaBi x As1‑x /GaAs multiple quantum wells

    NASA Astrophysics Data System (ADS)

    Balanta, M. A. G.; Kopaczek, J.; Orsi Gordo, V.; Santos, B. H. B.; Rodrigues, A. D.; Galeti, H. V. A.; Richards, R. D.; Bastiman, F.; David, J. P. R.; Kudrawiec, R.; Galvão Gobato, Y.

    2016-09-01

    Raman spectroscopy and magneto-photoluminescence measurements under high magnetic fields were used to investigate the optical and spin properties of GaBiAs/GaAs multiple quantum wells (MQWs). An anomalous negative diamagnetic energy shift was observed at higher temperatures and higher laser intensities, which was associated to a sign inversion of hole effective mass in these structures. In addition, an enhancement of the polarization degree with decreasing of laser intensity was observed (experimental condition where the emission is dominated by localized excitons). This effect was explained by changes of spin relaxation and exciton recombination times due to exciton localization by disorder.

  12. Exciton Emission under Strong Exciton-Plasmon Coupling in Carbon Nanotubes

    NASA Astrophysics Data System (ADS)

    Bondarev, Igor; Woods, Lilia; Tatur, Kevin

    2010-03-01

    We study theoretically the interactions of excitonic states with surface electromagnetic modes of small-diameter (˜1nm) semiconducting single-walled carbon nanotubes (CNs). We show that these interactions can result in strong exciton-interband-surface-plasmon coupling in individual CNs. This results in the exciton emission line (Rabi) splitting ˜0.1eV as the exciton energy is tuned to the nearest interband plasmon resonance of the CN [1]. The exciton-plasmon coupling strength we predict for individual CNs is close to that previously reported for hybrid plasmonic nanostructures artificially fabricated of organic semiconductors on metallic films [2]. The quantum confined Stark effect with an electrostatic field applied perpendicular to the CN axis can be used to control the exciton-plasmon coupling, and the exciton emission accordingly [3]. We expect this effect to open up paths to new tunable optoelectronic device applications of small-diameter semiconducting CNs.[4pt] [1] I.V.Bondarev, K.Tatur, L.M.Woods, Optics Commun. 282, 661 (2009). [2] J.Bellessa, et al., Phys. Rev. Lett. 93, 036404 (2004). [3] I.V.Bondarev, L.M.Woods, K.Tatur, Phys. Rev. B 80, 085407 (2009).

  13. Exciton-Exciton Annihilation in Copper-Phthalocyanine Single-Crystal Nanowires

    SciTech Connect

    Ma, Yingzhong; Xiao, Kai; Shaw, Robert W

    2012-01-01

    Femtosecond one-color pump-probe spectroscopy was applied to study exciton dynamics in single-crystal copper-phthalocyanine (CuPc) nanowires grown on an opaque silicon substrate. The transient reflectance kinetics measured at different pump fluences exhibit a remarkable intensity-dependent decay behavior which accelerates significantly with increasing pump pulse intensity. All the kinetic decays can be satisfactorily described using a bi-exponential decay function with lifetimes of 22 and 204 ps, and corresponding relative amplitudes depending on the pump intensity. The accelerated decay behavior observed at high pump intensities arises from a nonlinear exciton-exciton annihilation process. While this phenomenon has been found previously in crystalline metallophthalocyanine (MPc) polymorphs such as colloidal particles and thin films, the results obtained using the CuPc nanowires are markedly distinct, namely, much longer decay times and a linear intensity dependence of the initial peak amplitudes. Despite these differences, detailed data analysis further shows that, as found for other metal-phthalocyanine polymorphs, exciton-exciton annihilation in the CuPc nanowires is one-dimensional (1D) diffusion-limited, which possibly involves intra-chain exciton diffusion along 1D molecular stacks. The significantly long-lived excitons of CuPc nanowires in comparison to those of other crystalline polymorphs make them particularly suitable for photovoltaic applications.

  14. Microscopic theory of two-dimensional spatially-indirect-exciton condensates and exciton-polariton condensates

    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.

  15. Optically Detected Magnetic Resonance Studies on π-conjugated semiconductor systems

    SciTech Connect

    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 ΔmS=±1 and ΔmS=±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

  16. Probing Bose-Einstein condensation of excitons with electromagnetic radiation.

    PubMed

    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.

  17. Excitons in semiconducting superlattices, quantum wells, and ternary alloys

    SciTech Connect

    Sturge, M.D. ); Nahory, R.E.; Tamargo, M.C. )

    1991-08-15

    It is now possible to fabricate semiconducting layered structures with precisely defined layer thicknesses down to one monolayer (two atomic diameters). An example is the superlattice'' (SL) structure, in which two semiconductors with different band gaps are interleaved. The electronic properties of the SL are quite different from those of the constitutents and offer interesting new possibilities both in device design and in basic physics. This proposal aims to improve our understanding of optically excited states ( excitons'' and electron-hole plasmas'') in a particular class of these structures: the so-called Type 2 indirect'' SL's in which the electron and hole created by optical excitation are separated both in real and in momoentum space. Time-resolved tunable laser spectroscopy, with and without external perturbations such as magnetic field, electric field, and uniaxial stress, are used principally to study the following phenomena. 1. Exciton states in SLs with only a few atomic layers per period, for which the familiar effective mass model'' of semiconductor states breaks down. 2. The electron-hole plasma which forms when the excitation density is high. This plasma may be in a liquid state at low temperatures. In the short period superlattices are our primary concern, electrons and holes are spatially separated, leading to internal electric fields which might be expected to have a pronounced effect on the plasma properties.

  18. Harvesting excitons through plasmonic strong coupling

    NASA Astrophysics Data System (ADS)

    Gonzalez-Ballestero, Carlos; Feist, Johannes; Moreno, Esteban; Garcia-Vidal, Francisco J.

    2015-09-01

    Exciton harvesting is demonstrated in an ensemble of quantum emitters coupled to localized surface plasmons. When the interaction between emitters and the dipole mode of a metallic nanosphere reaches the strong-coupling regime, the exciton conductance is greatly increased. The spatial map of the conductance matches the plasmon field intensity profile, which indicates that transport properties can be tuned by adequately tailoring the field of the plasmonic resonance. Under strong coupling, we find that pure dephasing can have detrimental or beneficial effects on the conductance, depending on the effective number of participating emitters. Finally, we show that the exciton transport in the strong-coupling regime occurs on an ultrafast time scale given by the inverse Rabi splitting (˜10 fs), which is orders of magnitude faster than transport through direct hopping between the emitters.

  19. Possibility of observation of polaron normal modes at the far-infrared spectrum of acetanilide and related organics

    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.

  20. 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

  1. High-voltage thermionic polaron emission in the presence of adsorbed nonmetal nanofilm on a cathode

    NASA Astrophysics Data System (ADS)

    Barengolts, Yu. A.; Beril, S. I.

    2016-07-01

    The equation of thermionic emission has been derived, which takes into account the presence of thin films of adsorbed gas-environment molecules on a cathode under conditions of high-voltage gas discharge. It is shown that the consideration of electron polaron tunneling mechanism leads to a significant (by more than an order of magnitude) decrease in the emission-current density. A comparison with the classical Richardson-Schottky equation is performed. The role of the polaron effect is shown to strongly increase with an increase in the applied electric field strength and a decrease in temperature, which is due to an increase in the electron work function because of polaron nature.

  2. 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.

  3. Monte Carlo study of efficiency roll-off of phosphorescent organic light-emitting diodes: Evidence for dominant role of triplet-polaron quenching

    SciTech Connect

    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.

  4. Ab initio prediction of fast non-equilibrium transport of nascent polarons in SrI2: a key to high-performance scintillation [First-principles study of hole polaron formation and migration in strontium iodide

    DOE PAGES

    Zhou, Fei; Sadigh, Babak; Aberg, Daniel; Erhart, Paul

    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

  5. Arsenic-bound excitons in diamond

    NASA Astrophysics Data System (ADS)

    Barjon, J.; Jomard, F.; Morata, S.

    2014-01-01

    A set of new excitonic recombinations is observed in arsenic-implanted diamond. It is composed of two groups of emissions at 5.355/5.361 eV and at 5.215/5.220/5.227 eV. They are respectively attributed to the no-phonon and transverse-optical phonon-assisted recombinations of excitons bound to neutral arsenic donors. From the Haynes rule, an ionization energy of 0.41 eV is deduced for arsenic in diamond, which shows that arsenic is a shallower donor than phosphorus (0.6 eV), in agreement with theory.

  6. Exciton dynamics in perturbed vibronic molecular aggregates

    PubMed Central

    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

  7. Control of exciton transport using quantum interference

    NASA Astrophysics Data System (ADS)

    Lusk, Mark T.; Stafford, Charles A.; Zimmerman, Jeramy D.; Carr, Lincoln D.

    2015-12-01

    It is shown that quantum interference can be employed to create an exciton transistor. An applied potential gates the quasiparticle motion and also discriminates between quasiparticles of differing binding energy. When implemented within nanoscale assemblies, such control elements could mediate the flow of energy and information. Quantum interference can also be used to dissociate excitons as an alternative to using heterojunctions. A finite molecular setting is employed to exhibit the underlying discrete, two-particle, mesoscopic analog to Fano antiresonance. Selected entanglement measures are shown to distinguish regimes of behavior which cannot be resolved from population dynamics alone.

  8. 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.

  9. Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla

    DOE PAGES

    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 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

  10. 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.

  11. On the drift mobility of a molecular polaron in the presence of Coulomb traps

    NASA Astrophysics Data System (ADS)

    Rackovsky, S.; Scher, H.

    1999-08-01

    We study the drift mobility of a molecular polaron in the presence of an external applied field and Coulomb traps. The model is based on one previously developed for geminate recombination of photogenerated charge carriers. It is shown that the unusual combination of Poole-Frenkel-like field dependence and non-Arrhenius temperature dependence of the mobility, measured experimentally in molecular films, is well reproduced by this model. Our key result is that this nearly universal experimental behavior of the mobility arises from competition between rates of polaron trapping and release from a very low density of Coulomb traps.

  12. Electron Spin Resonance Spectra of Photogenerated Polarons in Poly(Paraphenylene Vinylene)

    NASA Astrophysics Data System (ADS)

    Murata, Kazuhiro; Kuroda, Shin-ichi; Shimoi, Yukihiro; Abe, Shuji; Noguchi, Takanobu; Ohnishi, Toshihiro

    1996-12-01

    Light-induced ESR (LESR) measurements have been performed on undoped poly(parapheny- lene vinylene) (PPV) down to 4 K. The ESR signal increases significantly for the excitation energy above 3.1 3.2 eV, as in the case of the excitation spectra of photocarriers reported in PPV derivatives. The anisotropic light-induced ESR spectra in oriented samples are well reproduced by the spectra calculated using a theoretical polaron spin distribution in the case of finite electron-electron interaction. These spectral features indicate that the observed spins are photogenerated polarons.

  13. Determination of free polaron lifetime in organic bulk heterojunction solar cells by transient time analysis

    SciTech Connect

    Li, Kejia; Shen, Yang; Majumdar, Nabanita; Hu, Chong; Gupta, Mool C.; Campbell, Joe C.

    2010-01-01

    A transient response technique that is widely used to measure the minority carrier lifetime in inorganic semiconductors is proposed to measure the lifetime of free polarons in a polymer:fullerene bulk heterojunction (BHJ) solar cell. A numerical model that can be used to describe the transient behavior of BHJ devices has been developed. Using the proposed method, the lifetime of free polarons in poly (3-hexylthiophene) and [6, 6]-phenyl C61-butyric acid methyl ester blend film is estimated to be in the range of 300–400 ns.

  14. Electronic structure and polaronic excitation in FeVO{sub 4}

    SciTech Connect

    Dixit, A.; Lawes, G.; Chen, P.; Musfeldt, J. L.

    2011-10-03

    We investigated the electronic properties of FeVO{sub 4} films using optical, valence band x-ray photoelectron, and infrared spectroscopies. These studies show that FeVO{sub 4} is a direct bandgap system with a 2.7 eV gap with the Fermi level in the middle of the valence band maximum and conduction band minimum. A polaronic excitation is also observed in the middle infrared, indicating the importance of charge-lattice coupling in this multiferroic material. Fits to a model for the optical response of large polarons yield a binding energy of approximately 130 meV.

  15. Inapplicability of small-polaron model for the explanation of infrared absorption spectrum in acetanilide.

    PubMed

    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. PMID:19811399

  16. Bright and dark excitons in semiconductor carbon nanotubes

    SciTech Connect

    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

  17. Exciton-exciton annihilation and relaxation pathways in semiconducting carbon nanotubes

    NASA Astrophysics Data System (ADS)

    Chmeliov, Jevgenij; Narkeliunas, Jonas; Graham, Matt W.; Fleming, Graham R.; Valkunas, Leonas

    2016-01-01

    We present a thorough analysis of one- and two-color transient absorption measurements performed on single- and double-walled semiconducting carbon nanotubes. By combining the currently existing models describing exciton-exciton annihilation--the coherent and the diffusion-limited ones--we are able to simultaneously reproduce excitation kinetics following both E11 and E22 pump conditions. Our simulations revealed the fundamental photophysical behavior of one-dimensional coherent excitons and non-trivial excitation relaxation pathways. In particular, we found that after non-linear annihilation a doubly-excited exciton relaxes directly to its E11 state bypassing the intermediate E22 manifold, so that after excitation resonant with the E11 transition, the E22 state remains unpopulated. A quantitative explanation for the observed much faster excitation kinetics probed at E22 manifold, comparing to those probed at the E11 band, is also provided.

  18. Polarization-dependent exciton linewidth in semiconductor quantum wells: A consequence of bosonic nature of excitons

    NASA Astrophysics Data System (ADS)

    Singh, Rohan; Suzuki, Takeshi; Autry, Travis M.; Moody, Galan; Siemens, Mark E.; Cundiff, Steven T.

    2016-08-01

    The exciton coherent signal decay rate in GaAs quantum wells, as measured in four-wave mixing experiments, depends on the polarization of the excitation pulses. Using polarization-dependent two-dimensional coherent spectroscopy, we show that this behavior is due to the bosonic character of excitons. Interference between two different quantum mechanical pathways results in a smaller decay rate for cocircular and colinear polarization of the optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a larger decay rate. Our result shows that the bosonic nature of excitons must be considered when interpreting ultrafast spectroscopic studies of exciton dephasing in semiconductors. This behavior should be considered while interpreting results of ultrafast spectroscopy experiments involving bosonlike excitations.

  19. Topological aspects of nonlinear excitonic processes in noncentrosymmetric crystals

    NASA Astrophysics Data System (ADS)

    Morimoto, Takahiro; Nagaosa, Naoto

    2016-07-01

    We study excitonic processes second order in the electric fields in noncentrosymmetric crystals. We derive formulas for shift current and second harmonic generation produced by exciton creation, by using the Floquet formalism combined with the Keldysh Green's function method. It is shown that (i) the steady dc shift current flows by exciton creation without dissociation into free carriers and (ii) second harmonic generation is enhanced at the exciton resonance. The obtained formulas clarify topological aspects of these second order excitonic processes which are described by Berry connections of the relevant valence and conduction bands.

  20. Exciton localization and drift in tailored-potential quantum nanowires

    SciTech Connect

    Szeszko, J. Rudra, A.; Kapon, E.; Belykh, V. V.; Sibeldin, N. N.

    2014-06-30

    Exciton recombination dynamics in tailored-potential, site-controlled AlGaAs quantum wires (QWRs) are studied. Time-resolved photoluminescence spectra evidence exciton localization in weakly disordered “uniform” QWRs, whereas deterministic bandgap grading is shown to suppress localization and promote exciton drift along the potential gradient. Measured exciton transit times between two quantum dot probes placed at opposite ends of the potential gradient yield the effective 1D exciton mobility as >1300 cm{sup 2}/(eVs).

  1. 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.

  2. Revealing the nature of excitons in liquid exfoliated monolayer tungsten disulphide.

    PubMed

    Kłopotowski, Ł; Backes, C; Mitioglu, A A; Vega-Mayoral, V; Hanlon, D; Coleman, J N; Ivanov, V Y; Maude, D K; Plochocka, P

    2016-10-21

    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. PMID:27606691

  3. Revealing the nature of excitons in liquid exfoliated monolayer tungsten disulphide.

    PubMed

    Kłopotowski, Ł; Backes, C; Mitioglu, A A; Vega-Mayoral, V; Hanlon, D; Coleman, J N; Ivanov, V Y; Maude, D K; Plochocka, P

    2016-10-21

    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.

  4. 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.

  5. Multiple Exciton Generation in Colloidal Silicon Nanocrystals

    SciTech Connect

    Beard, M. C.; Knutsen, K. P.; Yu, P.; Luther, J. M.; Song, Q.; Metzger, W. K.; Ellingson, R. J.; Nozik, A. M.

    2007-01-01

    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_to} Eg = 1.20 eV) to be 2.4 {+-} 0.1E{sub g} and find an exciton-production quantum yield of 2.6 {+-} 0.2 excitons per absorbed photon at 3.4E{sub g}. 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.

  6. Bias activated dielectric response of excitons and excitonic Mott transition in quantum confined lasers structures.

    NASA Astrophysics Data System (ADS)

    Bhunia, Amit; Bansal, Kanika; Datta, Shouvik; Alshammari, Marzook S.; Henini, Mohamed

    In contrast to the widely reported optical techniques, there are hardly any investigations on corresponding electrical signatures of condensed matter physics of excitonic phenomena. We studied small signal steady state capacitance response in III-V materials based multi quantum well (AlGaInP) and MBE grown quantum dot (InGaAs) laser diodes to identify signatures of excitonic presence. Conductance activation by forward bias was probed using frequency dependent differential capacitance response (fdC/df), which changes characteristically with the onset of light emission indicating the occurrence of negative activation energy. Our analysis shows that it is connected with a steady state population of exciton like bound states. Calculated average energy of this bound state matches well with the binding energy of weakly confined excitons in this type of structures. Further increase in charge injection decreases the differential capacitive response in AlGaInP based diodes, indicating a gradual Mott transition of excitonic states into electron hole plasma. This electrical description of excitonic Mott transition is fully supplemented by standard optical spectroscopic signatures of band gap renormalization and phase space filling effects.

  7. Magnetic and optical properties of Mn-doped ZnO vertically aligned nanorods synthesized by hydrothermal technique

    NASA Astrophysics Data System (ADS)

    Panda, J.; Sasmal, I.; Nath, T. K.

    2016-03-01

    In this paper we have reported the synthesis of high quality vertically aligned undoped and Mn-doped ZnO single crystalline nanorods arrays on Si (100) substrates using two steps process, namely, initial slow seed layer formation followed by solution growth employing wet chemical hydrothermal method. The shapes of the as grown single crystalline nanorods are hexagonal. The diameter and length of the as grown undoped ZnO nanorods varies in the range of 80-150 nm and 1.0 - 1.4 μm, respectively. Along with the lattice parameters of the hexagonal crystal structure, the diameter and length of Mn doped ZnO nanorods are found to increase slightly as compared to the undoped ZnO nanorods. The X-ray photoelectron spectroscopy confirms the presence of Mn atoms in Mn2+ state in the single crystalline ZnO nanorods. The recorded photoluminescence spectrum contains two emissions peaks having UV exciton emissions along with a green-yellow emission. The green-yellow emissions provide the evidence of singly ionized oxygen vacancies. The magnetic field dependent magnetization measurements [M (H)] and zero field cooled (ZFC) and field cooled (FC) magnetization [M(T)] measurements have been carried out at different isothermal conditions in the temperature range of 5-300 K. The Mn doped ZnO nanorods clearly show room temperature ferromagnetic ordering near room temperature down to 5 K. The observed magnetization may be attributed to the long range ferromagnetic interaction between bound magnetic polarons led by singly charged oxygen vacancies.

  8. Polaron pair mediated triplet generation in polymer/fullerene blends

    PubMed Central

    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

  9. 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.

  10. Influence of molecular designs on polaronic and vibrational transitions in a conjugated push-pull copolymer

    PubMed Central

    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

  11. 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.

  12. Small polarons and point defects in LaFeO3

    NASA Astrophysics Data System (ADS)

    Zhu, Zhen; Peelaers, Hartwin; van de Walle, Chris G.

    The proton-conductive perovskite-type LaFeO3 is a promising negative-electrode material for Ni/metal-hydride (Ni-MH) batteries. It has a discharge capacity up to 530 mAhg-1 at 333 K, which is significantly higher than commercialized AB5-type alloys. To elucidate the underlying mechanism of this performance, we have investigated the structural and electronic properties of bulk LaFeO3, as well as the effect of point defects, using hybrid density functional methods. LaFeO3 is antiferromagnetic in the ground state with a band gap of 3.54 eV. Small hole and electron polarons can form through self- or point-defect-assisted trapping. We find that La vacancies and Sr substitutional on La sites are shallow acceptors with the induced holes trapped as small polarons, while O and Fe vacancies are deep defect centers. Hydrogen interstitials behave like shallow donors, with the donor electrons localized on nearby iron sites as electron polarons. With a large trapping energy, these polarons can act as electron or hole traps and affect the electrical performance of LaFeO3 as the negative electrode for Ni-MH batteries. We acknowledge DOE for financial support.

  13. Charge reorganization energy and small polaron binding energy of rubrene thin films by ultraviolet photoelectron spectroscopy.

    PubMed

    Duhm, Steffen; Xin, Qian; Hosoumi, Shunsuke; Fukagawa, Hirohiko; Sato, Kazushi; Ueno, Nobuo; Kera, Satoshi

    2012-02-14

    The hole–phonon coupling of a rubrene monolayer on graphite is measured by means of angle resolved ultraviolet photoelectron spectroscopy. Thus, the charge reorganization energy λ and the small polaron binding energy is determined, which allows insight into the nature of charge transport in condensed rubrene. PMID:22403829

  14. Competition between polaron pair formation and singlet fission observed in amorphous rubrene films

    NASA Astrophysics Data System (ADS)

    Jankus, Vygintas; Snedden, Edward W.; Bright, Daniel W.; Arac, Erhan; Dai, DeChang; Monkman, Andrew P.

    2013-06-01

    In this paper, we investigate excited state dynamics in amorphous rubrene vacuum sublimed films. We report the direct observation of singlet fission in amorphous rubrene films. We have determined the fission rate to be >2.5×1012 s-1. Simultaneously, we observe strong polaron pair absorption and propose that polaron pair formation could be competing with singlet fission. Another possible conclusion from our experiments could be that two triplets from singlet fission might arise via polaron pairs. In either case, polaron pairs play an important role in singlet fission in an amorphous rubrene film. We also observe that triplets created by singlet fission fuse to regenerate a singlet, giving delayed fluorescence (DF) scaling linearly with initial laser energy (i.e., one singlet gives two triplets and two triplets give back one singlet). This is a strong evidence of S1n→2T1. We did not observe substantial temperature dependence of DF decay curve shape, indicating that triplet migration in amorphous rubrene films is not hopping limited and that triplets undergo fusion before their migration.

  15. Spin-flip Raman scattering of the neutral and charged excitons confined in a CdTe/(Cd,Mg)Te quantum well

    NASA Astrophysics Data System (ADS)

    Debus, J.; Dunker, D.; Sapega, V. F.; Yakovlev, D. R.; Karczewski, G.; Wojtowicz, T.; Kossut, J.; Bayer, M.

    2013-05-01

    Spin-flip Raman scattering of electrons and heavy holes is studied for resonant excitation of neutral and charged excitons in a CdTe/Cd0.63Mg0.37Te quantum well. The spin-flip scattering is characterized by its dependence on the incident and scattered light polarization as well as on the magnetic field strength and orientation. Model schemes of electric-dipole-allowed spin-flip Raman processes in the exciton complexes are compared to the experimental observations, from which we find that lowering the exciton symmetry, time of carrier spin relaxation, and mixing between electron states and, respectively, light- and heavy-hole states play an essential role in the scattering. At the exciton resonance, anisotropic exchange interaction induces heavy-hole spin-flip scattering, while acoustic phonon interaction is mainly responsible for the electron spin-flip. In resonance with the positively and negatively charged excitons, anisotropic electron-hole exchange as well as mixed electron states allow spin-flip scattering. Variations in the resonant excitation energy and lattice temperature demonstrate that localization of resident electrons and holes controls the Raman process probability and is also responsible for symmetry reduction. We show that the intensity of the electron spin-flip scattering is strongly affected by the lifetime of the exciton complex, and in tilted magnetic fields it is affected by the angular dependence of the anisotropic electron-hole exchange interaction.

  16. Ultrafast exciton dissociation followed by nongeminate charge recombination in PCDTBT:PCBM photovoltaic blends.

    PubMed

    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.

  17. Criteria for validating polaron pair dissociation in polymer-fullerene bulk heterojunction solar cells

    NASA Astrophysics Data System (ADS)

    Inche Ibrahim, M. L.

    2016-04-01

    The dissociation of polaron pairs into free charge carriers in organic bulk heterojunction solar cells is a fundamental step in generating photocurrent and is still in debate. In this study, we propose two simple criteria that can be used to test the validity of any polaron pair dissociation model for polymer-fullerene bulk heterojunction solar cells. The first criterion states that the ratio of the bimolecular recombination current density to the maximum photocurrent density should increase as a function of applied voltage. The second criterion states that the ratio of the bimolecular recombination current density to the maximum photocurrent density at short circuit should not be larger than 1. We apply these criteria to test the validity of the widely used Onsager-Braun model by using the experimental current-voltage data of poly[2-methoxy-5-(3'-7'-dimethyloctyloxy)-p-phenylene vinylene] (OC1C10-PPV) and [6,6]-phenyl C61-butyric acid methylester (PCBM) based solar cells. We find that our numerical analysis is not suitable to employ these criteria. Our analytical analysis, on the other hand, clearly demonstrates that the Onsager-Braun model simply cannot fulfill the first criteria. The reason is because the polaron pair dissociation given by the Onsager-Braun model is too strongly influenced by the electric field (i.e., decreases too rapidly as the electric field decreases). The analysis provides a further evidence against the widely used Onsager-Braun model. The proposed criteria can help us to determine the correct model for polaron pair dissociation by serving as a guideline on how strongly the electric field is allowed to influence the polaron pair dissociation.

  18. Final Report, DOE grant DE-FG02-99ER45780, "Indirect Excitons in Coupled Quantum Wells"

    SciTech Connect

    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.

  19. 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.

  20. 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.

  1. Short-lived charge-transfer excitons in organic photovoltaic cells studied by high-field magneto-photocurrent.

    PubMed

    Devir-Wolfman, Ayeleth H; Khachatryan, Bagrat; Gautam, Bhoj R; Tzabary, Lior; Keren, Amit; Tessler, Nir; Vardeny, Z Valy; Ehrenfreund, Eitan

    2014-07-29

    The main route of charge photogeneration in efficient organic photovoltaic cells based on bulk hetero-junction donor-acceptor blends involves short-lived charge-transfer excitons at the donor-acceptor interfaces. The cell efficiency is critically affected by the charge-transfer exciton recombination and dissociation processes. By measuring the magneto-photocurrent under ambient conditions at room temperature, we show here that magnetic field-induced spin-mixing among the charge-transfer exciton spin sublevels occurs in fields up to at least 8.5 Tesla. The resulting magneto-photocurrent increases at high fields showing non-saturating behaviour up to the highest applied field. We attribute the observed high-field spin-mixing mechanism to the difference in the donor-acceptor g-factors. The non-saturating magneto-photocurrent response at high field indicates that there exist charge-transfer excitons with lifetime in the sub-nanosecond time domain. The non-Lorentzian high-field magneto-photocurrent response indicates a dispersive decay mechanism that originates due to a broad distribution of charge-transfer exciton lifetimes.

  2. 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

  3. Optical properties of MgZnO alloys: Excitons and exciton-phonon complexes

    SciTech Connect

    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.

  4. Interlayer excitons with tunable dispersion relation

    NASA Astrophysics Data System (ADS)

    Skinner, Brian

    2016-06-01

    Interlayer excitons, comprising an electron in one material bound by Coulomb attraction to a hole in an adjacent material, are composite bosons that can assume a variety of many-body phases. The phase diagram of the bosonic system is largely determined by the dispersion relation of the bosons, which itself arises as a combination of the dispersion relations of the electron and hole separately. Here I show that in situations where either the electron or the hole has a nonmonotonic, "Mexican hat-shaped" dispersion relation, the exciton dispersion relation can have a range of qualitatively different forms, each corresponding to a different many-body phase at low temperature. This diversity suggests a platform for continuously tuning between different quantum phases using an external field.

  5. 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.

  6. Exciton Binding energies and effective masses in Organo-lead Tri-Halide Perovskites

    NASA Astrophysics Data System (ADS)

    Portugall, Oliver; Miyata, Atsuhiko; Mitioglu, Anatol; Plochocka, Paulina; Wang, Jacob Tse-Wei; Stranks, Samuel; Snaith, Henry; Nicholas, Robin; Lncmi Toulouse Team; Oxford University Team

    2015-03-01

    Solid-state perovskite-based solar cells have made a dramatic impact on emerging PV research with efficiencies of over 17% already achieved. However, to date the basic electronic properties of the perovskites such as the electron and hole effective masses and the exciton binding energy are not well known. We have measured both for methyl ammonium lead tri-iodide using magneto absorption in very high magnetic fields up to 150T showing that the exciton binding energy at low temperatures is only 16 meV, a value three times smaller than previously thought and sufficiently small to completely transform the way in which the devices must operate. Landau level spectroscopy shows that the reduced effective mass of 0.104 me is also smaller than previously thought. In addition by using a fast pulse 150T magnet we measure the band structure change due to the structural phase transition that occurs in this system at around 160K. We also observe Landau levels in the high temperature phase as used for device production, which has a very similar effective mass and the analysis suggests an exciton binding energy which is even smaller than in the low temperature phase.

  7. Excitonic Aharonov-Bohm effect in a two-dimensional quantum ring

    SciTech Connect

    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.

  8. Exciton-polariton oscillations in real space

    NASA Astrophysics Data System (ADS)

    Liew, T. C. H.; Rubo, Y. G.; Kavokin, A. V.

    2014-12-01

    We introduce and model spin-Rabi oscillations based on exciton-polaritons in semiconductor microcavities. The phase and polarization of oscillations can be controlled by resonant coherent pulses and the propagation of oscillating domains gives rise to phase-dependent interference patterns in real space. We show that interbranch polariton-polariton scattering controls the propagation of oscillating domains, which can be used to realize logic gates based on an analog variable phase.

  9. 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.

  10. Wannier-Mott excitons in semiconductors with a superlattice

    SciTech Connect

    Suris, R. A.

    2015-06-15

    The effect of the motion of a Wannier-Mott exciton in semiconductors with a superlattice formed by heterojunctions on the exciton binding energy and wave function is analyzed. This effect arises as a result of the fact that the dispersion laws of the electron and hole that form an exciton in a superlattice differ from the quadratic law. The investigated one-dimensional superlattice consists of alternating semiconductor layers with different energy positions of the conduction and valence bands, i.e., with one-dimensional wells and barriers. The exciton state in a superlattice consisting of quantum dots is analyzed. It is demonstrated that the closer the electron and hole effective masses, the greater the dependence of the binding energy on the exciton quasi-momentum. The possibility of replacing the tunneling excitation transfer between superlattice cells with the dipole-dipole one at certain exciton quasi-wave vector values is investigated.

  11. Energy levels of exciton in a gapped graphene sheet

    NASA Astrophysics Data System (ADS)

    Fallah, Farhang; Esmaeilzadeh, Mahdi

    2013-08-01

    A theory is presented for exciton formation in a graphene sheet using the center-of-mass approximation. The energy levels and wavefunctions of exciton are calculated analytically which show that the exciton can form if the band gap of graphene is not zero. We show that the energy gap of graphene plays the role of the mass which if not zero, leads to formation of the excitons. It is shown that the main quantum number of the exciton ground state changes with the graphene dielectric constant. Also, all of the states are found to be four-fold degenerate. The binding energy of exciton can reach as high as 1/4 of the energy gap of graphene which is notable among the conventional quasi-2D systems. This result can play an important rule in the photonics of graphene.

  12. Laser pulse induced multiple exciton kinetics in molecular ring structures

    NASA Astrophysics Data System (ADS)

    Hou, Xiao; Wang, Luxia

    2016-11-01

    Multiple excitons can be formed upon strong optical excitation of molecular aggregates and complexes. Based on a theoretical approach on exciton-exciton annihilation dynamics in supramolecular systems (May et al., 2014), exciton interaction kinetics in ring aggregates of two-level molecules are investigated. Excited by the sub-picosecond laser pulse, multiple excitons keep stable in the molecular ring shaped as a regular polygon. If the symmetry is destroyed by changing the dipole of a single molecule, the excitation of different molecules becomes not identical, and the changed dipole-dipole interaction initiates subsequent energy redistribution. Depending on the molecular distance and the dipole configuration, the kinetics undergo different types of processes, but all get stable within some hundreds of femtoseconds. The study of exciton kinetics will be helpful for further investigations of the efficiency of optical devices based on molecular aggregates.

  13. Singlet Exciton Fission in Nanostructured Organic Solar Cells

    SciTech Connect

    Jadhav, P. J.; Mohanty, A.; Sussman, J.; Baldo, Marc

    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{sub 6}0. 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{sub 60}. We measure a singlet fission efficiency of (71 ± 18)%, demonstrating that exciton fission can efficiently compete with exciton dissociation on the nanoscale.

  14. Fluorescence spectroscopy, exciton dynamics, and photochemistry of single allophycocyanin trimers

    SciTech Connect

    Ying, L.; Sie, X.S.

    1998-12-10

    The authors report a study of the allophycocyanin trimer (APC), a light-harvesting protein complex from cyanobacteria, by room-temperature single-molecule measurements of fluorescence spectra, lifetimes, intensity trajectories, and polarization modulation. Emission spectra of individual APC trimers are found to be homogeneous on the time scale of seconds. In contrast, their emission lifetimes are found to be widely distributed because of generation of long-lived exciton traps during the course of measurements. The intensity trajectories and polarization modulation experiments indicate reversible exciton trap formation within the three quasi-independent pairs of strong interacting {alpha}84 and {beta}84 chromophores in APC, as well as photobleaching of individual chromophores. Comparison experiments under continuous-wave and pulsed excitation reveal a two-photon mechanism for generating exciton traps and/or photobleaching, which involves exciton-exciton annihilation. These single-molecule experiments provide new insights into the spectroscopy, exciton dynamics, and photochemistry of light-harvesting complexes.

  15. Excitonic effects in oxyhalide scintillating host compounds

    SciTech Connect

    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.

  16. Fractional Solitons in Excitonic Josephson Junctions

    NASA Astrophysics Data System (ADS)

    Hsu, Ya-Fen; Su, Jung-Jung

    2015-10-01

    The Josephson effect is especially appealing to physicists because it reveals macroscopically the quantum order and phase. In excitonic bilayers the effect is even subtler due to the counterflow of supercurrent as well as the tunneling between layers (interlayer tunneling). Here we study, in a quantum Hall bilayer, the excitonic Josephson junction: a conjunct of two exciton condensates with a relative phase ϕ0 applied. The system is mapped into a pseudospin ferromagnet then described numerically by the Landau-Lifshitz-Gilbert equation. In the presence of interlayer tunneling, we identify a family of fractional sine-Gordon solitons which resemble the static fractional Josephson vortices in the extended superconducting Josephson junctions. Each fractional soliton carries a topological charge Q that is not necessarily a half/full integer but can vary continuously. The calculated current-phase relation (CPR) shows that solitons with Q = ϕ0/2π is the lowest energy state starting from zero ϕ0 - until ϕ0 > π - then the alternative group of solitons with Q = ϕ0/2π - 1 takes place and switches the polarity of CPR.

  17. Valley excitons in two-dimensional semiconductors

    SciTech Connect

    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.

  18. Valley excitons in two-dimensional semiconductors

    DOE PAGES

    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 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

  19. Excitons in semiconducting superlattices, quantum wells, and ternary alloys

    SciTech Connect

    Sturge, M.D. . Dept. of Physics); Nahory, R.E.; Tamargo, M.C. )

    1992-06-01

    Semiconducting layered structures can now be fabricated with precisely defined layer thicknesses down to one monolayer. An example is the superlattice'' (SL) structure, in which to semiconductors with different band gaps are interleaved. The electronic and optical properties of the SL are quite different from those of the constitutents and offer interesting new possibilities both in device design and in basic physics. This proposal aims to improve our understanding of optically excited states in SL's, particularly in the so-called Type 2 indirect'' SL's in which in electron and hole created by optical excitation are separated both in real and in momentum space. We study these structures by time-resolved tunable laser spectroscopy, with and without external perturbations such as magnetic field, electric field, and uniaxial stress. In SLs with only a few atomic layers per period the familiar effective mass model'' of semiconductor states breaks down. We have made precise optical experiments on well-characterized material to test current first principles'' calculations of the band structure. Our work under this grant has shown that the material we are using is of sufficiently high quality to test the theoretical predictions. Comparison of theory and experiment provides a new and sensitive probe of the interface quality on a fine scale. Statistical analysis of the temperature dependence of the exciton decay dynamics provides complementary information. From a careful study of the exciton spectra of the recently discovered mixed type 1- type 2 CdTe/CdZnTe SLs we have obtained the band offset at the CdTe/CdZnTe interface to unprecedented accuracy.

  20. Field-induced exciton condensation in LaCoO3

    PubMed Central

    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

  1. Exciton-exciton annihilation and biexciton stimulated emission in graphene nanoribbons.

    PubMed

    Soavi, Giancarlo; Dal Conte, Stefano; Manzoni, Cristian; Viola, Daniele; Narita, Akimitsu; Hu, Yunbin; Feng, Xinliang; Hohenester, Ulrich; Molinari, Elisa; Prezzi, Deborah; Müllen, Klaus; Cerullo, Giulio

    2016-03-17

    Graphene nanoribbons display extraordinary optical properties due to one-dimensional quantum-confinement, such as width-dependent bandgap and strong electron-hole interactions, responsible for the formation of excitons with extremely high binding energies. Here we use femtosecond transient absorption spectroscopy to explore the ultrafast optical properties of ultranarrow, structurally well-defined graphene nanoribbons as a function of the excitation fluence, and the impact of enhanced Coulomb interaction on their excited states dynamics. We show that in the high-excitation regime biexcitons are formed by nonlinear exciton-exciton annihilation, and that they radiatively recombine via stimulated emission. We obtain a biexciton binding energy of ≈ 250 meV, in very good agreement with theoretical results from quantum Monte Carlo simulations. These observations pave the way for the application of graphene nanoribbons in photonics and optoelectronics.

  2. Many-polaron description of impurities in a Bose-Einstein condensate in the weak-coupling regime

    SciTech Connect

    Casteels, W.; Devreese, J. T.; Tempere, J.

    2011-12-15

    The weak-coupling many-polaron formalism is applied to the case of the polaronic system consisting of impurities in a Bose-Einstein condensate. This allows investigating the ground-state properties and the response of the system to Bragg spectroscopy. Then, this theory is applied to the system of spin-polarized fermionic lithium-6 impurities in a sodium condensate. The Bragg spectrum reveals a peak that corresponds to the emission of Bogoliubov excitations. Both the ground-state properties and the response spectrum show that the polaronic effect vanishes at high densities. We also look at two possibilities to define the polaronic effective mass and observe that this results in a different quantitative behavior if multiple impurities are involved.

  3. Multiparticle Exciton Ionization in Shallow Doped Carbon Nanotubes.

    PubMed

    Sau, Jay D; Crochet, Jared J; Doorn, Stephen K; Cohen, Marvin L

    2013-03-21

    Shallow hole doping in small-diameter semiconducting carbon nanotubes with a valley degeneracy is predicted to result in the resonant ionization of excitons into free electron-hole pairs. This mechanism, which relies on the chirality of the electronic states, causes excitons to decay with high efficiencies where the rate scales as the square of the dopant density. Moreover, multiparticle exciton ionization can account for delocalized fluorescence quenching when a few holes per micrometer of tube length are present.

  4. Exciton Transport in a Bilayer Quantum Hall Superfluid

    NASA Astrophysics Data System (ADS)

    Eisenstein, J. P.; Finck, A. D. K.; Nandi, D.; Pfeiffer, L. N.; West, K. W.

    2013-08-01

    Bilayer quantum Hall systems at vT = 1 support an excitonic ground state. In addition to the usual charged quasiparticles, this system possesses a condensate degree of freedom: exciton transport. Detection of this neutral transport mode is facilitated by the use of the Corbino multiply-connected geometry in which charge transport is suppressed. We here summarize our recent experiments on Corbino devices which directly demonstrate exciton transport across the bulk of the incompressible vT = 1 quantum Hall state.

  5. Exciton annihilation in dye-sensitized nanocrystalline semiconductor films

    NASA Astrophysics Data System (ADS)

    Namekawa, Akihiro; Katoh, Ryuzi

    2016-08-01

    Exciton annihilation in dye-sensitized nanocrystalline semiconductor (Al2O3) films has been studied through laser-induced fluorescence spectroscopy. The relative quantum yield of the fluorescence decreases with increasing excitation light intensity, the indication being that exciton annihilation occurred. The rate constants of the annihilation were estimated for three dyes, N719, D149, and MK2, that are known to be sensitizing dyes for efficient dye-sensitized solar cells. The hopping time between dye molecules and the diffusion length of excitons within their lifetime were also estimated to facilitate discussion of the relevance of exciton annihilation to primary processes in dye-sensitized solar cells.

  6. Simulations of singlet exciton diffusion in organic semiconductors: a review

    SciTech Connect

    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.

  7. Polarization-dependent exciton dynamics in tetracene single crystals

    SciTech Connect

    Zhang, Bo; Zhang, Chunfeng Xu, Yanqing; Wang, Rui; He, Bin; Liu, Yunlong; Zhang, Shimeng; Wang, Xiaoyong; Xiao, Min

    2014-12-28

    We conduct polarization-dependent ultrafast spectroscopy to study the dynamics of singlet fission (SF) in tetracene single crystals. The spectrotemporal species for singlet and triplet excitons in transient absorption spectra are found to be strongly dependent on probe polarization. By carefully analyzing the polarization dependence, the signals contributed by different transitions related to singlet excitons have been disentangled, which is further applied to construct the correlation between dynamics of singlet and triplet excitons. The anisotropy of exciton dynamics provides an alternative approach to tackle the long-standing challenge in understanding the mechanism of singlet fission in organic semiconductors.

  8. Revealing and Characterizing Dark Excitons through Coherent Multidimensional Spectroscopy.

    PubMed

    Tollerud, Jonathan O; Cundiff, Steven T; Davis, Jeffrey A

    2016-08-26

    Dark excitons are of fundamental importance in a broad range of contexts but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify parity-forbidden and spatially indirect excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms, and coupling strengths. The observations of coherent coupling between these states and bright excitons hint at a role for a multistep process by which excitons in the barrier can relax into the quantum wells. PMID:27610881

  9. Exciton migration and quenching in poly(propylene imine) dendrimers

    NASA Astrophysics Data System (ADS)

    Minevičiūtė, I.; Gulbinas, V.; Franckevičius, M.; Vaišnoras, R.; Marcos, M.; Serrano, J. L.

    2009-05-01

    Exciton migration between chromophore groups of the poly(propylene imine) dendrimer in chloroform solution and in solid state has been investigated by means of the time-resolved fluorescence measurements. Fluorescence decay kinetics, dynamic band shift and the depolarization rate have been analyzed. Exciton migration in a single dendrimer was found to be slow in comparison with temperature-dependent chromophore reorientation time of 150-600 ps. In a solid state chromophore groups form collective excitonic states responsible for the dendrimer film fluorescence. Exciton migration and localization to the lowest energy sites within the distributed density of states take place on a subnanosecond-nanosecond time scale.

  10. Upconverted photoluminescence induced by radiative coupling between excitons

    NASA Astrophysics Data System (ADS)

    Matsuda, Takuya; Yokoshi, Nobuhiko; Ishihara, Hajime

    2016-04-01

    We propose an unconventional scheme of photoluminescence in a semiconductor thin film, where the nonlocal correlation between an excitonic wave and light wave prominently enhances the interaction between different excitonic states via radiation beyond the long-wavelength approximation (the so-called excitonic superradiance regime). On the basis of the developed method extending input-output theory, we elucidate atypical photoluminescence effects due to the strong wave-wave correlation. In particular, the upconverted photoluminescence based on the coherent quantum superposition of excitons is found to be highly efficient, i.e., it can be realized by weak pumping without auxiliary systems such as cavities or photonic antennas.

  11. Revealing and Characterizing Dark Excitons through Coherent Multidimensional Spectroscopy

    NASA Astrophysics Data System (ADS)

    Tollerud, Jonathan O.; Cundiff, Steven T.; Davis, Jeffrey A.

    2016-08-01

    Dark excitons are of fundamental importance in a broad range of contexts but are difficult to study using conventional optical spectroscopy due to their weak interaction with light. We show how coherent multidimensional spectroscopy can reveal and characterize dark states. Using this approach, we identify parity-forbidden and spatially indirect excitons in InGaAs/GaAs quantum wells and determine details regarding lifetimes, homogeneous and inhomogeneous linewidths, broadening mechanisms, and coupling strengths. The observations of coherent coupling between these states and bright excitons hint at a role for a multistep process by which excitons in the barrier can relax into the quantum wells.

  12. Binding energies of indirect excitons in double quantum well systems

    NASA Astrophysics Data System (ADS)

    Rossokhaty, Alex; Schmult, Stefan; Dietsche, Werner; von Klitzing, Klaus; Kukushkin, Igor

    2011-03-01

    A prerequisite towards Bose-Einstein condensation is a cold and dense system of bosons. Indirect excitons in double GaAs/AlGaAs quantum wells (DQWs) are believed to be suitable candidates. Indirect excitons are formed in asymmetric DQW structures by mass filtering, a method which does not require external electric fields. The exciton density and the electron-hole balance can be tuned optically. Binding energies are measured by a resonant microwave absorption technique. Our results show that screening of the indirect excitons becomes already relevant at densities as low as ~ 5 × 109 cm-2 and results in their destruction.

  13. Exciton management in organic photovoltaic multidonor energy cascades.

    PubMed

    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. PMID:24702468

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

    PubMed

    Guzelturk, Burak; Demir, Hilmi Volkan

    2015-06-18

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

  15. Excitonic Aharonov-Bohm effect in isotopically pure {sup 70}Ge/Si self-assembled type-II quantum dots

    SciTech Connect

    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.

  16. Renormalization group approach to the Fröhlich polaron model: application to impurity-BEC problem

    PubMed Central

    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

  17. Renormalization group approach to the Fröhlich polaron model: application to impurity-BEC problem.

    PubMed

    Grusdt, F; Shchadilova, Y E; Rubtsov, A N; Demler, E

    2015-07-17

    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.

  18. Temperature dependence of small polaron population decays in iron-doped lithium niobate by Monte Carlo simulations

    NASA Astrophysics Data System (ADS)

    Mhaouech, I.; Guilbert, L.

    2016-10-01

    The population decay of light-induced small polarons in iron-doped lithium niobate is simulated by a Monte-Carlo method on the basis of Holstein's theory. The model considers random walks of both bound polarons (NbLi4+) and free polarons (NbNb4+) ending to deep traps (FeLi3+). The thermokinetic interplay between polaron species is introduced by trapping and de-trapping rates at niobium antisites (NbLi). The decay of the NbLi4+ population proceeds by three possible channels: direct trapping at FeLi3+ sites, hopping on niobium antisites and hopping on Nb regular sites after conversion to the free state. Up to three regimes, each one reflecting the predominance of one of these processes, appear with different activation energies in the Arrhenius plots of the decay time. The influence of FeLi and NbLi concentrations on the transition temperatures is evidenced. For both polaron species, the length of the final hop (trapping length) is found much larger than the usual hopping length and decreases at rising temperature. This trap size effect is a natural consequence of Holstein's theory and may explain some unclear features of polaron-related light-induced phenomena, such as the temperature-dependent stretching exponent of light-induced absorption decays and the anomalous increase of the photoconductivity at high doping levels.

  19. Effect of Electron-Hole Overlap and Exchange Interaction on Exciton Radiative Lifetimes of CdTe/CdSe Heteronanocrystals.

    PubMed

    Granados Del Águila, Andrés; Groeneveld, Esther; Maan, Jan C; de Mello Donegá, Celso; Christianen, Peter C M

    2016-04-26

    Wave function engineering has become a powerful tool to tailor the optical properties of semiconductor colloidal nanocrystals. Core-shell systems allow to design the spatial extent of the electron (e) and hole (h) wave functions in the conduction- and valence bands, respectively. However, tuning the overlap between the e- and h-wave functions not only affects the oscillator strength of the coupled e-h pairs (excitons) that are responsible for the light emission, but also modifies the e-h exchange interaction, leading to an altered excitonic energy spectrum. Here, we present exciton lifetime measurements in a strong magnetic field to determine the strength of the e-h exchange interaction, independently of the e-h overlap that is deduced from lifetime measurements at room temperature. We use a set of CdTe/CdSe core/shell heteronanocrystals in which the electron-hole separation is systematically varied. We are able to unravel the separate effects of e-h overlap and e-h exchange on the exciton lifetimes, and we present a simple model that fully describes the recombination lifetimes of heteronanostructures (HNCs) as a function of core volume, shell volume, temperature, and magnetic fields. PMID:26982795

  20. Effect of Electron-Hole Overlap and Exchange Interaction on Exciton Radiative Lifetimes of CdTe/CdSe Heteronanocrystals.

    PubMed

    Granados Del Águila, Andrés; Groeneveld, Esther; Maan, Jan C; de Mello Donegá, Celso; Christianen, Peter C M

    2016-04-26

    Wave function engineering has become a powerful tool to tailor the optical properties of semiconductor colloidal nanocrystals. Core-shell systems allow to design the spatial extent of the electron (e) and hole (h) wave functions in the conduction- and valence bands, respectively. However, tuning the overlap between the e- and h-wave functions not only affects the oscillator strength of the coupled e-h pairs (excitons) that are responsible for the light emission, but also modifies the e-h exchange interaction, leading to an altered excitonic energy spectrum. Here, we present exciton lifetime measurements in a strong magnetic field to determine the strength of the e-h exchange interaction, independently of the e-h overlap that is deduced from lifetime measurements at room temperature. We use a set of CdTe/CdSe core/shell heteronanocrystals in which the electron-hole separation is systematically varied. We are able to unravel the separate effects of e-h overlap and e-h exchange on the exciton lifetimes, and we present a simple model that fully describes the recombination lifetimes of heteronanostructures (HNCs) as a function of core volume, shell volume, temperature, and magnetic fields.

  1. Laser assisted bound-free transition of a polaron bound to an impurity center

    NASA Astrophysics Data System (ADS)

    Sinha, C.; Biswas, R.; Mukhopadhyay, S.

    2013-12-01

    The scattering of a bound Frohlich large polaron in the presence of a coulomb impurity center as well as a linearly polarized laser field is studied. The differential (DCS) as well as the momentum transfer cross sections (MTCS) and the conductivity depend remarkably on the electron-phonon coupling (αP) and the strength of the coulomb impurity (β). The strongly bound polaron is found to be reluctant to contribute to the conductivity which is justified physically. The curves for MTCS and conductivity verses αP and β appear to be complementary, indicating the possibility of controlling the mobility and thereby conductivity by varying one of the parameters. This behavior indicates the possibility of optimizing the composition of optoelectronic materials where laser is the dominant source of excitation.

  2. Finite-temperature Wigner solid and other phases of ripplonic polarons on a helium film

    NASA Astrophysics Data System (ADS)

    Klimin, Serghei N.; Tempere, Jacques; Misko, Vyacheslav R.; Wouters, Michiel

    2016-07-01

    Electrons on liquid helium can form different phases depending on density, and temperature. Also the electron-ripplon coupling strength influences the phase diagram, through the formation of so-called "ripplonic polarons", that change how electrons are localized, and that shifts the transition between the Wigner solid and the liquid phase. We use an all-coupling, finite-temperature variational method to study the formation of a ripplopolaron Wigner solid on a liquid helium film for different regimes of the electron-ripplon coupling strength. In addition to the three known phases of the ripplopolaron system (electron Wigner solid, polaron Wigner solid, and electron fluid), we define and identify a fourth distinct phase, the ripplopolaron liquid. We analyse the transitions between these four phases and calculate the corresponding phase diagrams. This reveals a reentrant melting of the electron solid as a function of temperature. The calculated regions of existence of the Wigner solid are in agreement with recent experimental data.

  3. Translation invariant theory of polaron (bipolaron) and the problem of quantizing near the classical solution

    SciTech Connect

    Lakhno, V. D.

    2013-06-15

    A physical interpretation of translation-invariant polarons and bipolarons is presented, some results of their existence are discussed. Consideration is given to the problem of quantization in the vicinity of the classical solution in the quantum field theory. The lowest variational estimate is obtained for the bipolaron energy E({eta}) with E(0) = -0.440636{alpha}{sup 2}, where {alpha} is a constant of electron-phonon coupling, {eta} is a parameter of ion binding.

  4. Polaron Stabilization by Cooperative Lattice Distortion and Cation Rotations in Hybrid Perovskite Materials.

    PubMed

    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

    2016-06-01

    Solution-processed organometallic perovskites have rapidly developed into a top candidate for the active layer of photovoltaic devices. Despite 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. Here 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 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. 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. PMID:27224519

  5. Femtosecond dynamics of photogenerated solitons and polarons in trans-polyacetylene

    NASA Astrophysics Data System (ADS)

    Rothberg, L.; Jedju, T. M.; Townsend, P. D.; Etemad, S.; Baker, G. L.

    1990-07-01

    Intrachain and interchain excitations are clearly identified by polarized time-resolved absorption studies of photoinduced midgap bands in well-aligned trans-polyacetylene. We report spectroscopic evidence of the lattice deformation during intrachain photogeneration of charged soliton pairs, and see these pairs recombine geminatley in <2 ps. For incident polarization perpendicular to the chain direction, our data also show that interchain electron-hole pair excitation occurs with fairly high quantum yield and leads to polaron formation.

  6. 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.

  7. Polaron Stabilization by Cooperative Lattice Distortion and Cation Rotations in Hybrid Perovskite Materials.

    PubMed

    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

    2016-06-01

    Solution-processed organometallic perovskites have rapidly developed into a top candidate for the active layer of photovoltaic devices. Despite 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. Here 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 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. 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.

  8. Mapping polaronic states and lithiation gradients in individual V2O5 nanowires.

    PubMed

    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

    2016-06-28

    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.

  9. Photogeneration of superparaelectric large polarons in dielectrics with soft anharmonic T1u phonons

    NASA Astrophysics Data System (ADS)

    Nasu, Keiichiro

    2003-05-01

    In connection with the recent experiments on photoenhancements of the electronic conductivity and the quasistatic electric susceptibility of SrTiO3, we theoretically study global versus local parity violation of a photogenerated electron in this dielectric. The photogenerated electron, being quite itinerant in the 3d band of Ti, is assumed to couple weakly but quadratically with soft-anharmonic T1u phonons in this dielectric. The electron is also assumed to couple strongly but linearly to the breathing (A1g) type high energy phonons. We will show that these two types of electron-phonon (e-p) couplings result in two types of polarons, a “superparaelectric large polaron” with a quasiglobal parity violation, and an “off-center type self-trapped polaron” with only a local parity violation. These two states are shown to be separated by an adiabatic potential barrier, if these e-p couplings are short in their force ranges. Without the T1u phonon, these two states reduce to the well-known large polaron and the self-trapped one, both of which have even parities. We will also show that this superparaelectric large polaron enhances both the electronic conductivity and the quasistatic electric susceptibility, in qualitative agreements with the experiments.

  10. Structural correlations in the generation of polaron pairs in low-bandgap polymers for photovoltaics

    NASA Astrophysics Data System (ADS)

    Tautz, Raphael; da Como, Enrico; Limmer, Thomas; Feldmann, Jochen; Egelhaaf, Hans-Joachim; von Hauff, Elizabeth; Lemaur, Vincent; Beljonne, David; Yilmaz, Seyfullah; Dumsch, Ines; Allard, Sybille; Scherf, Ullrich

    2012-07-01

    Polymeric semiconductors are materials where unique optical and electronic properties often originate from a tailored chemical structure. This allows for synthesizing conjugated macromolecules with ad hoc functionalities for organic electronics. In photovoltaics, donor-acceptor co-polymers, with moieties of different electron affinity alternating on the chain, have attracted considerable interest. The low bandgap offers optimal light-harvesting characteristics and has inspired work towards record power conversion efficiencies. Here we show for the first time how the chemical structure of donor and acceptor moieties controls the photogeneration of polaron pairs. We show that co-polymers with strong acceptors show large yields of polaron pair formation up to 24% of the initial photoexcitations as compared with a homopolymer (η=8%). π-conjugated spacers, separating the donor and acceptor centre of masses, have the beneficial role of increasing the recombination time. The results provide useful input into the understanding of polaron pair photogeneration in low-bandgap co-polymers for photovoltaics.

  11. Mixed polaronic-ionic conduction in lithium borate glasses and glass-ceramics containing copper oxide

    NASA Astrophysics Data System (ADS)

    Khalil, M. M. I.

    2007-03-01

    The effect of electric field strength on conduction in lithium borate glasses doped with CuO with different concentration was studied and the value of the jump distance of charge carrier was calculated. The conductivity measurements indicate that the conduction is due to non-adiabatic hopping of polarons and the activation energies are found to be temperature and concentration dependent. Lithium borate glasses are subjected to carefully-programmed thermal treatments which cause the nucleation and growth of crystalline phases. X-ray diffraction analysis confirmed the amorphous nature for the investigated glass sample and the formation of crystalline phase for annealed samples at 650 °C. The main separated crystalline phase is Li2B8O13. The scanning electron micrographs of some selected glasses showed a significant change in the morphology of the films investigated due to heat treatment of the glass samples. It was found that the dc-conductivity decreases with an increase of the HT temperature. The decrease of dc conductivity, with an increase of the HT temperature, can be related to the decrease in the number of free ions in the glass matrix. There is deviation from linearity at high temperature regions in the logσ-1/T plots for all investigated doped samples at a certain temperature at which the transition from polaronic to ionic conduction occurs. The hopping of small polarons is dominant at low temperatures, whereas the hopping of Li+ ions dominates at high temperatures.

  12. Vast Hole- and Electron-Polaron Spatial Extent in Oligomeric π-Conjugated Porphyrin Arrays

    NASA Astrophysics Data System (ADS)

    Angiolillo, Paul; Rawson, Jeff; Therien, Michael

    meso-Ethyne bridged π-conjugated zinc porphyrin oligomers (PZnn compounds) have been demonstrated to evince lowest excited singlet states that are globally delocalized. It has also previously been shown that hole-polaron states of these oligomers exhibit delocalization lengths that mirror the molecular spatial dimension, 7.5 nm in the case of the heptamer. Here we demonstrate that the electron-polaron states in PZnn compounds also 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. These results are buttressed by electron spin relaxation measurements of PZnn electron polarons that show that both T1 and T2 relaxation times are unusually large, on the order of 103 ns and 102 ns, respectively. Since rapid charge delocalization defines an important mechanism that mitigates Coulombic stabilization of photogenerated electron-hole pairs to create separated free charge carriers, and spin polarization lifetimes feature prominently in spin currents, these findings identify conjugated materials with exceptional optical, electronic, and spintronic properties.

  13. 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.

  14. 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.

  15. Mapping polaronic states and lithiation gradients in individual V2O5 nanowires.

    PubMed

    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

    2016-01-01

    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. PMID:27349567

  16. Polaronic atom-trimer continuity in three-component Fermi gases.

    PubMed

    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.

  17. Excitonic luminescence upconversion in a two-dimensional semiconductor

    NASA Astrophysics Data System (ADS)

    Jones, Aaron M.; Yu, Hongyi; Schaibley, John R.; Yan, Jiaqiang; Mandrus, David G.; Taniguchi, Takashi; Watanabe, Kenji; Dery, Hanan; Yao, Wang; Xu, Xiaodong

    2016-04-01

    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. This phenomenon lies at the heart of optical refrigeration in solids, where upconversion relies on anti-Stokes processes enabled either by rare-earth impurities or exciton-phonon coupling. Here, 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. Since the charged exciton binding energy closely matches the 31 meV A1' optical phonon, 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. In addition, 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.

  18. Mapping the exciton diffusion in semiconductor nanocrystal solids.

    PubMed

    Kholmicheva, Natalia; Moroz, Pavel; Bastola, Ebin; Razgoniaeva, Natalia; Bocanegra, Jesus; Shaughnessy, Martin; Porach, Zack; Khon, Dmitriy; Zamkov, Mikhail

    2015-03-24

    Colloidal nanocrystal solids represent an emerging class of functional materials that hold strong promise for device applications. The macroscopic properties of these disordered assemblies are determined by complex trajectories of exciton diffusion processes, which are still poorly understood. Owing to the lack of theoretical insight, experimental strategies for probing the exciton dynamics in quantum dot solids are in great demand. Here, we develop an experimental technique for mapping the motion of excitons in semiconductor nanocrystal films with a subdiffraction spatial sensitivity and a picosecond temporal resolution. This was accomplished by doping PbS nanocrystal solids with metal nanoparticles that force the exciton dissociation at known distances from their birth. The optical signature of the exciton motion was then inferred from the changes in the emission lifetime, which was mapped to the location of exciton quenching sites. By correlating the metal-metal interparticle distance in the film with corresponding changes in the emission lifetime, we could obtain important transport characteristics, including the exciton diffusion length, the number of predissociation hops, the rate of interparticle energy transfer, and the exciton diffusivity. The benefits of this approach to device applications were demonstrated through the use of two representative film morphologies featuring weak and strong interparticle coupling.

  19. Storing excitons in transition-metal dichalcogenides using dark states

    NASA Astrophysics Data System (ADS)

    Gunlycke, Daniel; Tseng, Frank; Simsek, Ergun

    Monolayer transition-metal dichalcogenides exhibit strongly bound excitons confined to two dimensions. One challenge in exploiting these excitons is that they have a finite life time and collapse through electron-hole recombination. We propose that the exciton life time could be extended by transitioning the exciton population into dark states. The symmetry of these dark states require the electron and hole to be spatially separated, which not only causes these states to be optically inactive but also inhibits electron-hole recombination. Based on an atomistic model we call the Triangular Lattice Exciton (3ALE) model, we derive transition matrix elements and approximate selection rules showing that excitons could be transitioned into and out of dark states using a pulsed infrared laser. For illustration, we also present exciton population scenarios based on different recombination decay constants. Longer exciton lifetimes could make these materials candidates for applications in energy management and quantum information processing. This work was supported by the Office of Naval Research, directly and through the Naval Research Laboratory.

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

    PubMed

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

    2015-04-28

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

  1. Excitons in atomically thin black phosphorus

    NASA Astrophysics Data System (ADS)

    Surrente, A.; Mitioglu, A. A.; Galkowski, K.; Tabis, W.; Maude, D. K.; Plochocka, P.

    2016-03-01

    Raman scattering and photoluminescence spectroscopy are used to investigate the optical properties of single layer black phosphorus obtained by mechanical exfoliation of bulk crystals under an argon atmosphere. The Raman spectroscopy, performed in situ on the same flake as the photoluminescence measurements, demonstrates the single layer character of the investigated samples. The emission spectra, dominated by excitonic effects, display the expected in-plane anisotropy. The emission energy depends on the type of substrate on which the flake is placed due to the different dielectric screening. Finally, the blueshift of the emission with increasing temperature is well described using a two-oscillator model for the temperature dependence of the band gap.

  2. Feasibility study of a nuclear exciton laser

    NASA Astrophysics Data System (ADS)

    ten Brinke, Nicolai; Schützhold, Ralf; Habs, Dietrich

    2013-05-01

    Nuclear excitons known from Mössbauer spectroscopy describe coherent excitations of a large number of nuclei—analogous to Dicke states (or Dicke super-radiance) in quantum optics. In this paper, we study the possibility of constructing a laser based on these coherent excitations. In contrast to the free-electron laser (in its usual design), such a device would be based on stimulated emission and thus might offer certain advantages, e.g., regarding energy-momentum accuracy. Unfortunately, inserting realistic parameters, the window of operability is probably not open (yet) to present-day technology; but our design should be feasible in the UV regime, for example.

  3. 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.

  4. Spin–flip processes and radiative decay of dark intravalley excitons in transition metal dichalcogenide monolayers

    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.

  5. The excited spin-triplet state of a charged exciton in quantum dots.

    PubMed

    Molas, M R; Nicolet, A A L; Piętka, B; Babiński, A; Potemski, M

    2016-09-14

    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. PMID:27391126

  6. Spin-flip processes and radiative decay of dark intravalley excitons in transition metal dichalcogenide monolayers

    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.

  7. 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.

  8. Excitonic correlation in the Mott crossover regime in Ge

    NASA Astrophysics Data System (ADS)

    Sekiguchi, Fumiya; Shimano, Ryo

    2015-04-01

    Exciton Mott transition (EMT) in Ge was investigated by using optical-pump and terahertz-probe spectroscopy. From the quantitative analysis of optical conductivity and dielectric function, we evaluated the densities of unbound electron-hole pairs and excitons after the photoexcitation, from which we determined the ionization ratio of excitons α. The Mott crossover density region in Ge was elucidated from the density dependence of α in the temperature range above the critical temperature of electron-hole droplets. The 1 s -2 p excitonic transition energy hardly shifted with increasing density toward the EMT. Combined with the similar results recently observed in bulk Si, we suggest that the robustness of excitonic correlation against the Coulomb screening is a universal feature in bulk semiconductors in the Mott crossover regime.

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

    PubMed

    Zhu, X-Y

    2014-07-01

    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.

  10. 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

  11. Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla

    PubMed Central

    Stier, Andreas V.; McCreary, Kathleen M.; Jonker, Berend T.; Kono, Junichiro; Crooker, Scott A.

    2016-01-01

    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. PMID:26856412

  12. Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla.

    PubMed

    Stier, Andreas V; McCreary, Kathleen M; Jonker, Berend T; Kono, Junichiro; Crooker, Scott A

    2016-01-01

    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. PMID:26856412

  13. Exciton diamagnetic shifts and valley Zeeman effects in monolayer WS2 and MoS2 to 65 Tesla.

    PubMed

    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.

  14. Exciton Correlations in Intramolecular Singlet Fission.

    PubMed

    Sanders, Samuel N; Kumarasamy, Elango; Pun, Andrew B; Appavoo, Kannatassen; Steigerwald, Michael L; Campos, Luis M; Sfeir, Matthew Y

    2016-06-15

    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. PMID:27183040

  15. Exciton Dynamics in Semiconducting Carbon Nanotubes

    SciTech Connect

    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.

  16. Robust excitons inhabit soft supramolecular nanotubes

    PubMed Central

    Eisele, Dörthe M.; Arias, Dylan H.; Fu, Xiaofeng; Bloemsma, Erik A.; Steiner, Colby P.; Jensen, Russell A.; Rebentrost, Patrick; Eisele, Holger; Tokmakoff, Andrei; Lloyd, Seth; Nelson, Keith A.; Nicastro, Daniela; Knoester, Jasper; Bawendi, Moungi G.

    2014-01-01

    Nature's highly efficient light-harvesting antennae, such as those found in green sulfur bacteria, consist of supramolecular building blocks that self-assemble into a hierarchy of close-packed structures. In an effort to mimic the fundamental processes that govern nature’s efficient systems, it is important to elucidate the role of each level of hierarchy: from molecule, to supramolecular building block, to close-packed building blocks. Here, we study the impact of hierarchical structure. We present a model system that mirrors nature’s complexity: cylinders self-assembled from cyanine-dye molecules. Our work reveals that even though close-packing may alter the cylinders’ soft mesoscopic structure, robust delocalized excitons are retained: Internal order and strong excitation-transfer interactions—prerequisites for efficient energy transport—are both maintained. Our results suggest that the cylindrical geometry strongly favors robust excitons; it presents a rational design that is potentially key to nature’s high efficiency, allowing construction of efficient light-harvesting devices even from soft, supramolecular materials. PMID:25092336

  17. Exciton Correlations in Intramolecular Singlet Fission

    DOE PAGES

    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,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

  18. Coherent coupling of magneto-excitons probed by two-dimensional Fourier transform spectroscopy

    NASA Astrophysics Data System (ADS)

    Paul, Jagannath; Liu, Cunming; McGill, Stephen; Hilton, David; Karaiskaj, Denis

    We present the coherent two dimensional Fourier Transform (2DFT) spectra of magneto-excitons in undoped GaAs quantum wells at high magnetic field up to 10 Tesla. The 2DFT data reveal strong coherent coupling between resonances and line shapes which are strikingly different from the zero field spectra. 2DFT spectra measured using co-linear and co-circular polarizations at low temperatures will be discussed. The work at USF and UAB was supported by the National Science Foundation under Grant Number DMR-1409473. The work at NHMFL, Florida State University was supported by the National Science Foundation under Grant Numbers DMR-1157490 and DMR-1229217.

  19. Coherent transport and manipulation of spins in indirect-exciton nanostructures

    NASA Astrophysics Data System (ADS)

    Violante, A.; Hey, R.; Santos, P. V.

    2015-03-01

    We report on the coherent control and transport of indirect-exciton (IX) spins in GaAs double quantum well (DQW) nanostructures. The spin dynamics was investigated by optically generating spins using a focused, circularly polarized light spot and by probing their spatial distribution using spatially and polarization resolved photoluminescence spectroscopy. Optically injected IX spins precess while moving over distances exceeding 20 μ m from the excitation spot with a precession length that depends on the spin transport direction as well as on the bias applied across the DQW structure. This behavior is attributed to the spin precession in the effective magnetic field induced by the spin-orbit interaction. From the dependence of the spin dynamics on the transport direction, bias, and external magnetic fields we directly determined the Dresselhaus and Rashba electron spin splitting coefficients for the DQW structure. The precession dynamics is essentially independent of the IX density, thus indicating that the long spin lifetimes are not associated with IX collective effects. The long IX lifetimes, together with the negligible contribution of holes to the spin dynamics, are rather attributed to spatial separation of the electron and hole wave functions by the electric field, which reduces the electron-hole exchange interaction. If extended to the single-exciton regime, the present results on coherent spin precession over long transport distances as well as the control of the spin vector using electric and magnetic fields open the way for the application of IX spins in quantum information processing.

  20. Energy Transfer of Excitons Between Quantum Wells Separated by a Wide Barrier

    SciTech Connect

    LYO,SUNGKWUN K.

    1999-12-06

    We present a microscopic theory of the excitonic Stokes and anti-Stokes energy transfer mechanisms between two widely separated unequal quantum wells with a large energy mismatch ({Delta}) at low temperatures (T). Exciton transfer through dipolar coupling, photon-exchange coupling and over-barrier ionization of the excitons through exciton-exciton Auger processes are examined. The energy transfer rate is calculated as a function of T and the center-to-center distance d between the two wells. The rates depend sensitively on T for plane-wave excitons. For located excitons, the rates depend on T only through the T-dependence of the localization radius.

  1. Exciton Transfer in Carbon Nanotube Aggregates for Energy Harvesting Applications

    NASA Astrophysics Data System (ADS)

    Davoody, Amirhossein; Karimi, Farhad; Knezevic, Irena

    Carbon nanotubes (CNTs) are promising building blocks for organic photovoltaic devices, owing to their tunable band gap, mechanical and chemical stability. We study intertube excitonic energy transfer between pairs of CNTs with different orientations and band gaps. The optically bright and dark excitonic states in CNTs are calculated by solving the Bethe-Salpeter equation. We calculate the exciton transfer rates due to the direct and exchange Coulomb interactions, as well as the second-order phonon-assisted processes. We show the importance of phonons in calculating the transfer rates that match the measurements. In addition, we discuss the contribution of optically inactive excited states in the exciton transfer process, which is difficult to determine experimentally. Furthermore, we study the effects of sample inhomogeneity, impurities, and temperature on the exciton transfer rate. The inhomogeneity in the CNT sample dielectric function can increase the transfer rate by about a factor of two. We show that the exciton confinement by impurities has a detrimental effect on the transfer rate between pairs of similar CNTs. The exciton transfer rate increases monotonically with increasing temperature. Support by the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under Award DE-SC0008712.

  2. Excitons in InP/InAs inhomogeneous quantum dots

    NASA Astrophysics Data System (ADS)

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

    2003-01-01

    Wannier excitons confined in an InP/InAs inhomogeneous quantum dot (IQD) have been studied theoretically in the framework of the effective mass approximation. A finite-depth potential well has been used to describe the effect of the quantum confinement in the InAs layer. The exciton binding energy has been determined using the Ritz variational method. The spatial correlation between the electron and the hole has been taken into account in the expression for the wavefunction. It has been shown that for a fixed size b of the IQD, the exciton binding energy depends strongly on the core radius a. Moreover, it became apparent that there are two critical values of the core radius, acrit and a2D, for which important changes of the exciton binding occur. The former critical value, acrit, corresponds to a minimum of the exciton binding energy and may be used to distinguish between tridimensional confinement and bidimensional confinement. The latter critical value, a2D, corresponds to a maximum of the exciton binding energy and to the most pronounced bidimensional character of the exciton.

  3. 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.

  4. Hybrid em wave - polar semiconductor interaction: A polaronic study

    SciTech Connect

    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.

  5. Excitonic fine structure and binding energies of excitonic complexes in single InAs quantum dashes

    NASA Astrophysics Data System (ADS)

    Mrowiński, P.; Zieliński, M.; Świderski, M.; Misiewicz, J.; Somers, A.; Reithmaier, J. P.; Höfling, S.; Sek, G.

    2016-09-01

    The fundamental electronic and optical properties of elongated InAs nanostructures embedded in quaternary InGaAlAs barrier are investigated by means of high-resolution optical spectroscopy and many-body atomistic tight-binding theory. These wire-like shaped, self-assembled nanostructures are known as quantum dashes and are typically formed during the molecular beam epitaxial growth on InP substrates. In this paper, we study properties of excitonic complexes confined in quantum dashes emitting in a broad spectral range from below 1.2 to 1.55 μm. We find peculiar trends for the biexciton and negative trion binding energies, with pronounced trion binding in smaller size quantum dashes. These experimental findings are then compared and qualitatively explained by atomistic theory. The theoretical analysis shows a fundamental role of correlation effects for the absolute values of excitonic binding energies. Eventually, we determine the bright exciton fine structure splitting (FSS), where both the experiment and theory predict a broad distribution of the splitting varying from below 50 to almost 180 μeV. We identify several key factors determining the FSS values in such nanostructures, including quantum dash size variation and composition fluctuations.

  6. Excitonic AND Logic Gates on DNA Brick Nanobreadboards

    PubMed Central

    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

  7. Intraband effects in excitonic second-harmonic generation

    NASA Astrophysics Data System (ADS)

    Pedersen, Thomas Garm

    2015-12-01

    A theory for the nonlinear excitonic optical response of semiconductors is developed. By adopting the length gauge, intraband effects are rigorously taken into account. We show that the second-order nonlinear response mixing intra- and interband transitions can be expressed in terms of generalized derivatives of the exciton Green's function. The theory is applied to hexagonal boron-nitride monolayers. For both the linear and nonlinear response, a dramatic influence of excitons is found. Hence, new discrete resonances appear as well as pronounced changes in the continuum spectrum.

  8. Confocal shift interferometry of coherent emission from trapped dipolar excitons

    SciTech Connect

    Repp, J.; Schinner, G. J.; Schubert, E.; Rai, A. K.; Wieck, A. D.; Reuter, D.; Wurstbauer, U.; Holleitner, A. W.; and others

    2014-12-15

    We introduce a confocal shift-interferometer based on optical fibers. The presented spectroscopy allows measuring coherence maps of luminescent samples with a high spatial resolution even at cryogenic temperatures. We apply the spectroscopy onto electrostatically trapped, dipolar excitons in a semiconductor double quantum well. We find that the measured spatial coherence length of the excitonic emission coincides with the point spread function of the confocal setup. The results are consistent with a temporal coherence of the excitonic emission down to temperatures of 250 mK.

  9. Excitons and the lifetime of organic semiconductor devices

    PubMed Central

    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

  10. Ubiquity of Exciton Localization in Cryogenic Carbon Nanotubes

    PubMed Central

    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

  11. Ubiquity of Exciton Localization in Cryogenic Carbon Nanotubes.

    PubMed

    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.

  12. Spectroscopy of excitonic Zeeman levels in single quantum dots

    NASA Astrophysics Data System (ADS)

    Schaller, A.; Zrenner, A.; Abstreiter, G.; Böhm, G.

    1998-07-01

    Fully confined excitons are investigated in natural quantum dots, which are formed by well-width fluctuations in GaAs/AlAs coupled quantum-well structures. In magnetooptic experiments a population inversion of the Zeeman split levels in the quantum dots is found under the condition of charge injection from the AlAs X-point state. This new phenomenon is explained in terms of spin thermalization in the intermediate indirect exciton state and subsequent tunnelling into the direct quantum-dot state. Population inversion is thereby caused by the associated sign reversal of the effective exciton g-factor.

  13. Exciton coupling of surface complexes on a nanocrystal surface.

    PubMed

    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.

  14. Role of phonons in Josephson oscillations of excitonic and polaritonic condensates

    SciTech Connect

    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.

  15. Exciton and multi-exciton dynamics in CdSe/Cd1-xZnxS quantum dots

    NASA Astrophysics Data System (ADS)

    Righetto, Marcello; Minotto, Alessandro; Bozio, Renato

    2016-04-01

    The outstanding optical properties of Semiconductor Quantum Dots (QDs) have attracted much interest for over two decades. The development of synthetic methods for the production of core-shell QDs has opened the way to attaining almost ideal emitting properties. Their implementation in opto-electronic devices, such as light emitting diodes (LEDs) and lasers, requires a full understanding of the fine details of their photophysics. The exciton dynamics of core and coreshell QDs was extensively studied by means of pump and probe (P and P) and transient photoluminescence (TRPL) spectroscopies. Nevertheless, the wealth of possible exciton and multi-exciton decay mechanisms, operating on comparable time-scales, results in complex signals. In this work, the exciton dynamics of a complete CdSe/Cd1-xZnxS series is investigated, with a focus on exciton trapping processes. Insights into the energy distribution of exciton traps are unveiled by wavelength resolve QY measurements. Multicolor P and P measurements give a deeper insight into the dynamics of exciton trapping and Auger recombinations. An inversion method is proposed as a powerful tool for separating different contribution in complex P and P transients. The outcomes of this work clarify the role of core/shell interfaces and surfaces in modulating the optical properties and suggest possible routes for their improvement.

  16. Exciton-exciton annihilation in a disordered molecular system by direct and multistep Förster transfer

    NASA Astrophysics Data System (ADS)

    Fennel, Franziska; Lochbrunner, Stefan

    2015-10-01

    Exciton annihilation dynamics in a disordered organic model system is investigated by ultrafast absorption spectroscopy. We show that the temporal evolution of the exciton density can be quantitatively understood by applying Förster energy transfer theory to describe the diffusion of the excitons as well as the annihilation step itself. To this end, previous formulations of Förster theory are extended to account for the inhomogeneous distribution of the S0-S1 transition energies resulting in an effective exciton diffusion constant. Two annihilation pathways are considered, the direct transfer of an exciton between two excited molecules and diffusive motion by multiple transfer steps towards a second exciton preceding the annihilation event. One pathway can be emphasized with respect to the other by tuning the exciton diffusion constant via the chromophore concentration. The investigated system allows one to extract all relevant parameters for the description and provides in this way a proof that the annihilation dynamics can be entirely understood and modeled by Förster energy transfer.

  17. 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

  18. Luttinger liquid of polarons in one-dimensional boson-fermion mixtures.

    PubMed

    Mathey, L; Wang, D-W; Hofstetter, W; Lukin, M D; Demler, Eugene

    2004-09-17

    We use the bosonization approach to investigate quantum phases of boson-fermion mixtures (BFM) of atoms confined to one dimension by an anisotropic optical lattice. For a BFM with a single species of fermions we find a charge-density wave phase, a fermion pairing phase, and a phase separation regime. We also obtain the rich phase diagram of a BFM with two species of fermions. We demonstrate that these phase diagrams can be understood in terms of polarons, i.e., atoms "dressed" by screening clouds of the other atom species. Techniques to detect the resulting quantum phases are discussed.

  19. 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.

  20. Polaron hopping in some biomolecular solids and their charge transfer complexes.

    PubMed

    Solanki, G K; Amin, Anand; Padhiyar, Ashvin; Ray, A K; Oza, A T

    2008-12-01

    The solid state spectroscopy of charge transfer complexes of biomolecules such as fatty acids, tripalmitin, lysozyme. folic acid, beta-carotene, cytochrome c, valinomycin and gramicidin has been carried out. The absorption coefficient is related with electronic conductivity. A half-power beta density is found common among these macromolecular solids, indicating photon-induced polaron hopping or hopping of a charge carrier between two branches of a polariton. Band gap vs full width at half-maximum of the mid-IR peak also reveals a linear relation.

  1. Electron spin resonance and electron nuclear double resonance of photogenerated polarons in polyfluorene and its fullerene composite

    NASA Astrophysics Data System (ADS)

    Marumoto, K.; Kato, M.; Kondo, H.; Kuroda, S.; Greenham, N. C.; Friend, R. H.; Shimoi, Y.; Abe, S.

    2009-06-01

    Electron spin resonance (ESR) and electron-nuclear double resonance (ENDOR) of photogenerated polarons in poly(9,9-dioctylfluorene) (PFO) and its composite with fullerene (C60) using variable photoexcitation energy up to 4.1 eV are reported. For PFO, a light-induced ESR (LESR) signal (g=2.003) is observed below 60 K, and its transient response and excitation spectrum indicate that the observed spins are photogenerated polarons on PFO. For the PFO-C60 composite, two LESR signals of photogenerated positive polarons on PFO (g1=2.003) and radical anions on C60 (g2=1.999) , respectively, are observed below 120 K, which are caused by photoinduced electron transfer from PFO to C60 . A remarkable enhancement of the LESR signals in the excitation spectrum at ˜2.8eV is observed compared with the case of pure PFO. The bimolecular-recombination kinetics of photogenerated charge carriers in the composite are confirmed by the dependence of the LESR on excitation-light intensity and by the decay dynamics. Light-induced ENDOR (LENDOR) signals are clearly observed for excitation around 2.8 eV owing to the highly efficient photoinduced electron transfer in the composite. Broad LENDOR shifts directly reflect the spin-density distribution of the polarons in PFO. We have determined its maximum shift using LENDOR-induced ESR, and have evaluated the maximum spin density on the carbon site coupled to the proton as 0.032. This value is consistent with the theoretical result obtained by Pariser-Parr-Pople (PPP) model, where the spatial extent of the polarons is calculated as ˜3 monomer units of PFO. The calculated LESR spectra of PFO based on the PPP model are consistent with the experimental spectra, which confirm the above spatial extension of the polaron in PFO.

  2. 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.

  3. Exciton-polariton localized wave packets in a microcavity

    NASA Astrophysics Data System (ADS)

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

    2016-06-01

    We investigate the possibility of creating X waves, or localized wave packets, in resonantly excited exciton-polariton superfluids. We demonstrate the existence of X-wave traveling solutions in the coupled exciton-photon system past the inflection point, where the effective mass of lower polaritons is negative in the direction perpendicular to the wave vector of the pumping beam. Contrary to the case of bright solitons, X waves do not require nonlinearity for sustaining their shape. Nevertheless, we show that nonlinearity is important for their dynamics, as it allows for their spontaneous formation from an initial Gaussian wave packet. Unique properties of exciton-polaritons may lead to applications of their X waves in long-distance signal propagation inside novel integrated optoelectronic circuits based on excitons.

  4. Simulations of singlet exciton diffusion in organic semiconductors: a review

    DOE PAGES

    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

  5. Charge Transfer Excitons at van der Waals Interfaces.

    PubMed

    Zhu, Xiaoyang; Monahan, Nicholas R; Gong, Zizhou; Zhu, Haiming; Williams, Kristopher W; Nelson, Cory A

    2015-07-01

    The van der Waals interfaces of molecular donor/acceptor or graphene-like two-dimensional (2D) semiconductors are central to concepts and emerging technologies of light-electricity interconversion. Examples include, among others, solar cells, photodetectors, and light emitting diodes. A salient feature in both types of van der Waals interfaces is the poorly screened Coulomb potential that can give rise to bound electron-hole pairs across the interface, i.e., charge transfer (CT) or interlayer excitons. Here we address common features of CT excitons at both types of interfaces. We emphasize the competition between localization and delocalization in ensuring efficient charge separation. At the molecular donor/acceptor interface, electronic delocalization in real space can dictate charge carrier separation. In contrast, at the 2D semiconductor heterojunction, delocalization in momentum space due to strong exciton binding may assist in parallel momentum conservation in CT exciton formation. PMID:26001297

  6. Hopping approach towards exciton dissociation in conjugated polymers

    SciTech Connect

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

    2008-06-14

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

  7. Effect of correlation of local fluctuations on exciton coherence

    SciTech Connect

    Chen, Xin; Silbey, Robert J.

    2010-01-01

    Recent experimental studies have shown both oscillations of exciton populations and long lasting coherence in multichromophoric systems such as photosynthetic light harvesting systems and conjugated polymers. It has been suggested that this quantum effect is due to correlations of the fluctuations of site energies among the closely packed chromophores in the protein environment. In addition to these, there is the strong possibility of correlations between site energies and transfer matrix elements. In order to understand the role of such correlations we generalize the Haken–Strobl–Reineker (HSR) model to include the energetic correlations and the site diagonal-off-diagonal correlations in a systematic way. The extended HSR model in the exciton basis is also constructed and allows us to study the dynamics of the exciton populations and coherences. With the extended model, we can provide insight into how these correlations affect the evolution of the populations and coherences of excitons by comparing to the original HSR model with uncorrelated fluctuating environments.

  8. Strong Quantum Coherence between Fermi Liquid Mahan Excitons.

    PubMed

    Paul, J; Stevens, C E; Liu, C; Dey, P; McIntyre, C; Turkowski, V; Reno, J L; Hilton, D J; Karaiskaj, D

    2016-04-15

    In modulation doped quantum wells, the excitons are formed as a result of the interactions of the charged holes with the electrons at the Fermi edge in the conduction band, leading to the so-called "Mahan excitons." The binding energy of Mahan excitons is expected to be greatly reduced and any quantum coherence destroyed as a result of the screening and electron-electron interactions. Surprisingly, we observe strong quantum coherence between the heavy hole and light hole excitons. Such correlations are revealed by the dominating cross-diagonal peaks in both one-quantum and two-quantum two-dimensional Fourier transform spectra. Theoretical simulations based on the optical Bloch equations where many-body effects are included phenomenologically reproduce well the experimental spectra. Time-dependent density functional theory calculations provide insight into the underlying physics and attribute the observed strong quantum coherence to a significantly reduced screening length and collective excitations of the many-electron system.

  9. Quantum confinement of excitons in wurtzite InP nanowires

    NASA Astrophysics Data System (ADS)

    Pemasiri, K.; Jackson, H. E.; Smith, L. M.; Wong, B. M.; Paiman, S.; Gao, Q.; Tan, H. H.; Jagadish, C.

    2015-05-01

    Exciton resonances are observed in photocurrent spectra of 80 nm wurtzite InP nanowire devices at low temperatures, which correspond to transitions between the A, B, and C valence bands and the lower conduction band. Photocurrent spectra for 30 nm WZ nanowires exhibit shifts of the exciton resonances to higher energy, which are consistent with finite element calculations of wavefunctions of the confined electrons and holes for the various bands.

  10. Quantum confinement of excitons in wurtzite InP nanowires

    SciTech Connect

    Pemasiri, K.; Jackson, H. E.; Smith, L. M.; Wong, B. M.; Paiman, S.; Gao, Q.; Tan, H. H.; Jagadish, C.

    2015-05-21

    Exciton resonances are observed in photocurrent spectra of 80 nm wurtzite InP nanowire devices at low temperatures, which correspond to transitions between the A, B, and C valence bands and the lower conduction band. Photocurrent spectra for 30 nm WZ nanowires exhibit shifts of the exciton resonances to higher energy, which are consistent with finite element calculations of wavefunctions of the confined electrons and holes for the various bands.

  11. Kekule-distortion-induced exciton instability in graphene

    SciTech Connect

    Dillenschneider, Raoul

    2008-09-15

    Effects of a Kekule distortion on exciton instability in single-layer graphene are discussed. In the framework of quantum electrodynamics the mass of the electron generated dynamically is worked out using a Schwinger-Dyson equation. For homogeneous lattice distortion it is shown that the generated mass is independent of the amplitude of the lattice distortion at the one-loop approximation. Formation of excitons induced by the homogeneous Kekule distortion could appear only through direct dependence of the lattice distortion.

  12. Probing the origin of excitonic states in monolayer WSe2

    NASA Astrophysics Data System (ADS)

    Huang, Jiani; Hoang, Thang B.; Mikkelsen, Maiken H.

    2016-03-01

    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.

  13. Simulation of Singlet Exciton Diffusion in Bulk Organic Materials.

    PubMed

    Kranz, Julian J; Elstner, Marcus

    2016-09-13

    We present a scheme for nonadiabatic direct dynamics simulation of Frenkel exciton diffusion in bulk molecular systems. The fluctuations of exciton couplings caused by the molecular motion can crucially influence exciton transport in such materials. This effect can be conveniently taken into account by computing the exciton couplings along molecular dynamics trajectories, as shown recently. In this work, we combine Molecular Dynamics simulations with a Frenkel Hamiltonian into a combined quantum-mechanical/molecular mechanics approach in order to allow for a simultaneous propagation of nuclear and electronic degrees of freedom using nonadiabatic dynamics propagation schemes. To reach the necessary time and length scales, we use classical force-fields and the semiempirical time-dependent density functional tight-binding method in combination with a fragmentation of the electronic structure. Fewest-switches surface-hopping, with adaptions to handle trivial crossings, and the Boltzmann-corrected Ehrenfest method are used to follow the excitonic quantum dynamics according to the classical evolution of the nuclei. As an application, we present the simulation of singlet exciton diffusion in crystalline anthracene, which allows us to address strengths and shortcomings of the presented methodology in detail. PMID:27434173

  14. Probing the origin of excitonic states in monolayer WSe2.

    PubMed

    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

  15. Femtosecond THz Studies of Intra-Excitonic Transitions

    SciTech Connect

    Huber, Rupert; Schmid, Ben A.; Kaindl, Robert A.; Chemla, Daniel S.

    2007-10-02

    Few-cycle THz pulses are employed to resonantly access the internal fine structure of photogenerated excitons in semiconductors, on the femtosecond time scale. This technique allows us to gain novel insight into many-body effects of excitons and reveal key quantum optical processes. We discuss experiments that monitor the density-dependent re?normalization of the binding energy of a high-density exciton gas in GaAs/AlGaAs quantum wells close to the Mott transition. In a dilute ensemble of 3p excitons in Cu2O, stimulated THz emission from internal transitions to the energetically lower 2s state is observed at a photon energy of 6.6 meV, with a cross section of 10-14 cm2. Simultaneous interband excitation of both exciton levels drives quantum beats, which cause efficient THz emission at the difference frequency. By extending this principle to various other exciton resonances, we develop a novel way of mapping the fine structure by two-dimensional THz emission spectroscopy.

  16. Trapping and transport of indirect excitons in coupled quantum wells

    NASA Astrophysics Data System (ADS)

    Wuenschell, Jeffrey K.

    Spatially indirect excitons are optically generated composite bosons with a radiative lifetime sufficient to reach thermal equilibrium. This work explores the physics of indirect excitons in coupled quantum wells in the GaAs/AlGaAs system, specifically in the low-temperature, high-density regime. Particular attention is paid to a technique whereby a spatially inhomogeneous strain field is used as a trapping potential. In the process of modeling the trapping profile in wide quantum wells, dramatic effects due to intersubband coupling were observed at high strain. Experimentally, this regime coincides with the abrupt appearance of a dark population of indirect excitons at trap center, an effect originally suspected to be related to Bose-Einstein condensation. Here, the role of band mixing due to the strain-induced distortion of the crystal symmetry will be explored in detail in the context of this effect. Experimental studies presented here and in the literature suggest that Bose-Einstein condensation in indirect exciton systems may be difficult to detect with optical means (e.g., coherence measurements, momentum-space narrowing), possibly due to the strong dipole interaction between indirect excitons. Due to similarities between this system and liquid helium, it may be more fruitful to look for transport-related signatures of condensation, such as super fluidity. Here, a method for performing transport measurements on optically generated indirect excitons is also outlined and preliminary results are presented.

  17. Analysis of Triplet Exciton Loss Pathways in PTB7:PC71BM Bulk Heterojunction Solar Cells

    PubMed Central

    Kraus, Hannes; Heiber, Michael C.; Väth, Stefan; Kern, Julia; Deibel, Carsten; Sperlich, Andreas; Dyakonov, Vladimir

    2016-01-01

    A strategy for increasing the conversion efficiency of organic photovoltaics has been to increase the VOC by tuning the energy levels of donor and acceptor components. However, this opens up a new loss pathway from an interfacial charge transfer state to a triplet exciton (TE) state called electron back transfer (EBT), which is detrimental to device performance. To test this hypothesis, we study triplet formation in the high performing PTB7:PC71BM blend system and determine the impact of the morphology-optimizing additive 1,8-diiodoctane (DIO). Using photoluminescence and spin-sensitive optically detected magnetic resonance (ODMR) measurements at low temperature, we find that TEs form on PC71BM via intersystem crossing from singlet excitons and on PTB7 via EBT mechanism. For DIO blends with smaller fullerene domains, an increased density of PTB7 TEs is observed. The EBT process is found to be significant only at very low temperature. At 300 K, no triplets are detected via ODMR, and electrically detected magnetic resonance on optimized solar cells indicates that TEs are only present on the fullerenes. We conclude that in PTB7:PC71BM devices, TE formation via EBT is impacted by fullerene domain size at low temperature, but at room temperature, EBT does not represent a dominant loss pathway. PMID:27380928

  18. Analysis of Triplet Exciton Loss Pathways in PTB7:PC71BM Bulk Heterojunction Solar Cells

    NASA Astrophysics Data System (ADS)

    Kraus, Hannes; Heiber, Michael C.; Väth, Stefan; Kern, Julia; Deibel, Carsten; Sperlich, Andreas; Dyakonov, Vladimir

    2016-07-01

    A strategy for increasing the conversion efficiency of organic photovoltaics has been to increase the VOC by tuning the energy levels of donor and acceptor components. However, this opens up a new loss pathway from an interfacial charge transfer state to a triplet exciton (TE) state called electron back transfer (EBT), which is detrimental to device performance. To test this hypothesis, we study triplet formation in the high performing PTB7:PC71BM blend system and determine the impact of the morphology-optimizing additive 1,8-diiodoctane (DIO). Using photoluminescence and spin-sensitive optically detected magnetic resonance (ODMR) measurements at low temperature, we find that TEs form on PC71BM via intersystem crossing from singlet excitons and on PTB7 via EBT mechanism. For DIO blends with smaller fullerene domains, an increased density of PTB7 TEs is observed. The EBT process is found to be significant only at very low temperature. At 300 K, no triplets are detected via ODMR, and electrically detected magnetic resonance on optimized solar cells indicates that TEs are only present on the fullerenes. We conclude that in PTB7:PC71BM devices, TE formation via EBT is impacted by fullerene domain size at low temperature, but at room temperature, EBT does not represent a dominant loss pathway.

  19. Analysis of Triplet Exciton Loss Pathways in PTB7:PC71BM Bulk Heterojunction Solar Cells.

    PubMed

    Kraus, Hannes; Heiber, Michael C; Väth, Stefan; Kern, Julia; Deibel, Carsten; Sperlich, Andreas; Dyakonov, Vladimir

    2016-07-06

    A strategy for increasing the conversion efficiency of organic photovoltaics has been to increase the VOC by tuning the energy levels of donor and acceptor components. However, this opens up a new loss pathway from an interfacial charge transfer state to a triplet exciton (TE) state called electron back transfer (EBT), which is detrimental to device performance. To test this hypothesis, we study triplet formation in the high performing PTB7:PC71BM blend system and determine the impact of the morphology-optimizing additive 1,8-diiodoctane (DIO). Using photoluminescence and spin-sensitive optically detected magnetic resonance (ODMR) measurements at low temperature, we find that TEs form on PC71BM via intersystem crossing from singlet excitons and on PTB7 via EBT mechanism. For DIO blends with smaller fullerene domains, an increased density of PTB7 TEs is observed. The EBT process is found to be significant only at very low temperature. At 300 K, no triplets are detected via ODMR, and electrically detected magnetic resonance on optimized solar cells indicates that TEs are only present on the fullerenes. We conclude that in PTB7:PC71BM devices, TE formation via EBT is impacted by fullerene domain size at low temperature, but at room temperature, EBT does not represent a dominant loss pathway.

  20. Analysis of Triplet Exciton Loss Pathways in PTB7:PC71BM Bulk Heterojunction Solar Cells.

    PubMed

    Kraus, Hannes; Heiber, Michael C; Väth, Stefan; Kern, Julia; Deibel, Carsten; Sperlich, Andreas; Dyakonov, Vladimir

    2016-01-01

    A strategy for increasing the conversion efficiency of organic photovoltaics has been to increase the VOC by tuning the energy levels of donor and acceptor components. However, this opens up a new loss pathway from an interfacial charge transfer state to a triplet exciton (TE) state called electron back transfer (EBT), which is detrimental to device performance. To test this hypothesis, we study triplet formation in the high performing PTB7:PC71BM blend system and determine the impact of the morphology-optimizing additive 1,8-diiodoctane (DIO). Using photoluminescence and spin-sensitive optically detected magnetic resonance (ODMR) measurements at low temperature, we find that TEs form on PC71BM via intersystem crossing from singlet excitons and on PTB7 via EBT mechanism. For DIO blends with smaller fullerene domains, an increased density of PTB7 TEs is observed. The EBT process is found to be significant only at very low temperature. At 300 K, no triplets are detected via ODMR, and electrically detected magnetic resonance on optimized solar cells indicates that TEs are only present on the fullerenes. We conclude that in PTB7:PC71BM devices, TE formation via EBT is impacted by fullerene domain size at low temperature, but at room temperature, EBT does not represent a dominant loss pathway. PMID:27380928

  1. Madelung and Hubbard interactions in polaron band model of doped organic semiconductors.

    PubMed

    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

  2. Polaron absorption for photovoltaic energy conversion in a manganite-titanate pn heterojunction

    NASA Astrophysics Data System (ADS)

    Saucke, Gesine; Norpoth, Jonas; Jooss, Christian; Su, Dong; Zhu, Yimei

    2012-04-01

    The relation among structure, electric transport, and photovoltaic effect is investigated for a pn heterojunction with strong correlation interactions. A perovskite interface is chosen as a model system consisting of the p-doped strongly correlated manganite Pr0.64Ca0.36MnO3 (PCMO) and the n-doped titanate SrTi1-yNbyO3 (y=0.002 and 0.01). High-resolution electron microscopy and spectroscopy reveal a nearly dislocation-free, epitaxial interface and give insight into the local atomic and electronic structure. The presence of a photovoltaic effect under visible light at room temperature suggests the existence of mobile excited polarons within the band-gap-free PCMO absorber. The temperature-dependent rectifying current-voltage characteristics prove to be mainly determined by the presence of an interfacial energy spike in the conduction band and are affected by the colossal electroresistance effect. From the comparison of photocurrents and spatiotemporal distributions of photogenerated carriers (deduced from optical absorption spectroscopy), we discuss the range of the excited polaron diffusion length.

  3. Ideal Diode Equation for Organic Heterojunctions. II. The Role of Polaron Pair Recombination

    SciTech Connect

    Giebink, Noel C; Wiederrecht, Gary P; Wasielewski, Michael R; Forrest, Stephen R.

    2010-10-04

    In paper I [N. C. Giebink, G. P. Wiederrecht, M. R. Wasielewski, and S. R. Forrest, Phys. Rev. B 82, 155305 (2010)], we proposed that current transport in a donor-acceptor heterojunction (HJ) depends on the balance of polaron pair (PP) dissociation and recombination. Here, we directly investigate these processes in archetype planar copper phthalocyanine (CuPc)/C{sub 60} and boron subpthalocyanine chloride (SubPc)/C{sub 60} HJs. Using intensity-modulated photocurrent spectroscopy (IMPS) along with emission from interfacial Pc/C{sub 60} exciplex states, we monitor the geminate PP density at the HJ as a function of bias and illumination intensity. We find that the SubPc/C{sub 60} PP density is limited by the dynamics of dissociation, where it increases from short circuit, and peaks at open circuit. In contrast, that of CuPc/C{sub 60} is dominated by faster recombination kinetics and declines monotonically over the same voltage domain. We conclude that the PP recombination rate depends on electric field, and propose a simple expression that qualitatively explains the observed exciplex luminescence and IMPS behavior for these HJs. Our results provide insight into polaron pair recombination, which governs the current-voltage characteristics of organic heterojunctions in the dark and under illumination.

  4. Ideal diode equation for organic heterojunctions. II. The role of polaron pair recombination

    SciTech Connect

    Giebink, Noel C; Lassiter, Brian E; Wiederrecht, Gary P; Wasielewski, Michael R; Forrest, Stephen R.

    2010-10-04

    In paper I [N. C. Giebink, G. P. Wiederrecht, M. R. Wasielewski, and S. R. Forrest, Phys. Rev. B 82, 155305 (2010)], we proposed that current transport in a donor-acceptor heterojunction (HJ) depends on the balance of polaron pair (PP) dissociation and recombination. Here, we directly investigate these processes in archetype planar copper phthalocyanine (CuPc)/C{sub 60} and boron subpthalocyanine chloride (SubPc)/C{sub 60} HJs. Using intensity-modulated photocurrent spectroscopy (IMPS) along with emission from interfacial Pc/C{sub 60} exciplex states, we monitor the geminate PP density at the HJ as a function of bias and illumination intensity. We find that the SubPc/C{sub 60} PP density is limited by the dynamics of dissociation, where it increases from short circuit, and peaks at open circuit. In contrast, that of CuPc/C{sub 60} is dominated by faster recombination kinetics and declines monotonically over the same voltage domain. We conclude that the PP recombination rate depends on electric field, and propose a simple expression that qualitatively explains the observed exciplex luminescence and IMPS behavior for these HJs. Our results provide insight into polaron pair recombination, which governs the current-voltage characteristics of organic heterojunctions in the dark and under illumination.

  5. Polyaniline emeraldine salt in the amorphous solid state: polaron versus bipolaron.

    PubMed

    Canales, Manel; Torras, Juan; Fabregat, Georgina; Meneguzzi, Alvaro; Alemán, Carlos

    2014-10-01

    The polaronic and bipolaronic forms of polyaniline emeraldine salt (PAni-ES) in the amorphous solid state have been simulated using classical molecular dynamics (MD) and hybrid quantum mechanical/molecular mechanical-molecular dynamics (QM/MM-MD) approaches. It should be remarked that the electronic state of PAni-ES has been theoretically investigated in the gas phase, solution phase, and crystalline state, but this is the first study in the amorphous solid state, which is the most typical for this conducting polymer. MD simulations were carried out using force-field parametrizations explicitly developed for polaronic and bipolaronic models. QM/MM-MD calculations were performed using a quantum mechanical zone defined by four repeat units. In addition of the structural and electronic characteristics of the two forms of PAni-ES, MD and QM/MM-MD simulations indicate that the bipolaronic is the most stable state of amorphous PAni-ES. Complementary studies have been carried out using different experimental techniques. Although the morphology and topography of doped and undoped PAni are very similar, comparison of their UV-vis spectra supports the preference toward the bipolaronic form of PAni-ES.

  6. Electrochromism and small-polaron hopping in oxygen deficient and lithium intercalated amorphous tungsten oxide films

    NASA Astrophysics Data System (ADS)

    Triana, C. A.; Granqvist, C. G.; Niklasson, G. A.

    2015-07-01

    Thin films of Li x WO 3 - z with 0 ≤ x ≤ 0.27 and 0 ≤ z ≤ 0.27 were prepared by sputter deposition followed by electrochemical lithiation. Kramers-Kronig-consistent complex dielectric functions were obtained for these films by numerical inversion of experimental spectra of optical transmittance and reflectance by using a superposition of Tauc-Lorentz and Lorentz oscillator models. Low-energy optical absorption bands were induced by oxygen vacancies and/or by electrochemical intercalation of Li+ species together with charge compensating electrons. The experimental optical conductivity was fitted to a small-polaron model for disordered systems with strong electron-phonon interaction, taking into account transitions near the Fermi level. The optical absorption is due to small-polaron hopping and associated with the formation of W5+ states due to transfer of electrons from oxygen vacancies and/or insertion of Li+ species. The results also show increases in the Fermi level, caused by oxygen deficiency or Li+ insertion, which occur along with a band gap shift towards higher energies for the Li+ intercalated films.

  7. Anisotropic small-polaron hopping in W:BiVO{sub 4} single crystals

    SciTech Connect

    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.

  8. Polaronic transport and current blockades in epitaxial silicide nanowires and nanowire arrays.

    PubMed

    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. PMID:23902411

  9. Polaronic transport and current blockades in epitaxial silicide nanowires and nanowire arrays.

    PubMed

    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.

  10. Madelung and Hubbard interactions in polaron band model of doped organic semiconductors

    NASA Astrophysics Data System (ADS)

    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.

    2016-09-01

    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.

  11. Madelung and Hubbard interactions in polaron band model of doped organic semiconductors

    PubMed Central

    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

  12. Madelung and Hubbard interactions in polaron band model of doped organic semiconductors.

    PubMed

    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

    2016-09-01

    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.

  13. Exciton-dominant electroluminescence from a diode of monolayer MoS{sub 2}

    SciTech Connect

    Ye, Yu; Ye, Ziliang; Gharghi, Majid; Zhu, Hanyu; Wang, Yuan; Zhao, Mervin; Yin, Xiaobo; Zhang, Xiang

    2014-05-12

    In two-dimensional monolayer MoS{sub 2}, excitons dominate the absorption and emission properties. However, the low electroluminescent efficiency and signal-to-noise ratio limit our understanding of the excitonic behavior of electroluminescence. Here, we study the microscopic origin of the electroluminescence from a diode of monolayer MoS{sub 2} fabricated on a heavily p-type doped silicon substrate. Direct and bound-exciton related recombination processes are identified from the electroluminescence. At a high electron-hole pair injection rate, Auger recombination of the exciton-exciton annihilation of the bound exciton emission is observed at room temperature. Moreover, the efficient electrical injection demonstrated here allows for the observation of a higher energy exciton peak of 2.255 eV in the monolayer MoS{sub 2} diode, attributed to the excited exciton state of a direct-exciton transition.

  14. Room-Temperature Transport of Indirect Excitons in (Al ,Ga )N /GaN Quantum Wells

    NASA Astrophysics Data System (ADS)

    Fedichkin, F.; Guillet, T.; Valvin, P.; Jouault, B.; Brimont, C.; Bretagnon, T.; Lahourcade, L.; Grandjean, N.; Lefebvre, P.; Vladimirova, M.

    2016-07-01

    We report on the exciton propagation in polar (Al ,Ga )N /GaN quantum wells over several micrometers and up to room temperature. The key ingredient to achieve this result is the crystalline quality of GaN quantum wells grown on GaN substrate that limits nonradiative recombination. From the comparison of the spatial and temporal dynamics of photoluminescence, we conclude that the propagation of excitons under continuous-wave excitation is assisted by efficient screening of the in-plane disorder. Modeling within drift-diffusion formalism corroborates this conclusion and suggests that exciton propagation is still limited by the exciton scattering on defects rather than by exciton-exciton scattering so that improving interface quality can boost exciton transport further. Our results pave the way towards room-temperature excitonic devices based on gate-controlled exciton transport in wide-band-gap polar heterostructures.

  15. Cooperative Singlet and Triplet Exciton Transport in Tetracene Crystals Visualized by Ultrafast Microscopys

    SciTech Connect

    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.

  16. The influence of built-in electric field on binding energy of bound polaron and polaron effects in wurtzite ZnO/MgxZn1-xO quantum well

    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

  17. Negative activation energy and dielectric signatures of excitons and excitonic Mott transitions in quantum confined laser structures

    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.

  18. Experimental methods of post-growth tuning of the excitonic fine structure splitting in semiconductor quantum dots

    PubMed Central

    2012-01-01

    Deterministic sources of polarization entangled photon pairs on demand are considered as important building blocks for quantum communication technology. It has been demonstrated that semiconductor quantum dots (QDs), which exhibit a sufficiently small excitonic fine structure splitting (FSS) can be used as triggered, on-chip sources of polarization entangled photon pairs. As-grown QDs usually do not have the required values of the FSS, making the availability of post-growth tuning techniques highly desired. This article reviews the effect of different post-growth treatments and external fields on the FSS such as thermal annealing, magnetic fields, the optical Stark effect, electric fields, and anisotropic stress. As a consequence of the tuning of the FSS, for some tuning techniques a rotation of the polarization of the emitted light is observed. The joint modification of polarization orientation and FSS can be described by an anticrossing of the bright excitonic states. PMID:22726724

  19. Probing excitonic dark states in single-layer tungsten disulphide.

    PubMed

    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

  20. Fermi polaron in a one-dimensional quasiperiodic optical lattice: The simplest many-body localization challenge

    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.

  1. Exciton dynamics in individual semimagnetic (Zn,Mn)Te/(Zn,Mg)Te nanowires

    SciTech Connect

    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.

  2. Dark High Density Dipolar Liquid of Excitons

    NASA Astrophysics Data System (ADS)

    Cohen, Kobi; Shilo, Yehiel; West, Ken; Pfeiffer, Loren; Rapaport, Ronen

    2016-06-01

    The possible phases and the nano-scale particle correlations of two-dimensional interacting dipolar particles is a long-sought problem in many-body physics. Here we observe a spontaneous condensation of trapped two-dimensional dipolar excitons with internal spin degrees of freedom from an interacting gas into a high density, closely packed liquid state made mostly of dark dipoles. Another phase transition, into a bright, highly repulsive plasma is observed at even higher excitation powers. The dark liquid state is formed below a critical temperature $T_c \\approx 4.8K$, and it is manifested by a clear spontaneous spatial condensation to a smaller and denser cloud, suggesting an attractive part to the interaction which goes beyond the purely repulsive dipole-dipole forces. Contributions from quantum mechanical fluctuations are expected to be significant in this strongly correlated, long living dark liquid. This is a new example of a two-dimensional atomic-like interacting dipolar quantum liquid, but where the coupling of light to its internal spin degrees of freedom plays a crucial role in the dynamical formation and the nature of resulting ground state.

  3. Photosynthetic light harvesting: excitons and coherence

    PubMed Central

    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

  4. Photosynthetic light harvesting: excitons and coherence.

    PubMed

    Fassioli, Francesca; Dinshaw, Rayomond; Arpin, Paul C; Scholes, Gregory D

    2014-03-01

    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.

  5. Plasmon transmission through excitonic subwavelength gaps.

    PubMed

    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. PMID:27083741

  6. Dark High Density Dipolar Liquid of Excitons.

    PubMed

    Cohen, Kobi; Shilo, Yehiel; West, Ken; Pfeiffer, Loren; Rapaport, Ronen

    2016-06-01

    The possible phases and the nanoscale particle correlations of two-dimensional interacting dipolar particles is a long-sought problem in many-body physics. Here we observe a spontaneous condensation of trapped two-dimensional dipolar excitons with internal spin degrees of freedom from an interacting gas into a high density, closely packed liquid state made mostly of dark dipoles. Another phase transition, into a bright, highly repulsive plasma, is observed at even higher excitation powers. The dark liquid state is formed below a critical temperature Tc ≈ 4.8 K, and it is manifested by a clear spontaneous spatial condensation to a smaller and denser cloud, suggesting an attractive part to the interaction which goes beyond the purely repulsive dipole-dipole forces. Contributions from quantum mechanical fluctuations are expected to be significant in this strongly correlated, long living dark liquid. This is a new example of a two-dimensional atomic-like interacting dipolar liquid, but where the coupling of light to its internal spin degrees of freedom plays a crucial role in the dynamical formation and the nature of resulting condensed dark ground state.

  7. Chirality inversion in the bilirubin molecular exciton.

    PubMed

    Boiadjiev, S E; Lightner, D A

    2001-05-15

    The bichromophoric pigment bilirubin acts as a molecular exciton in its UV-visible and circular dichroism (CD) spectroscopy. In both polar and nonpolar solvents, an optically active analog, (beta R,beta 'R)-dimethylmesobilirubin-XIII alpha (1), exhibits intense bisignate CD Cotton effects in the region of its long wavelength UV-vis absorption near 400 nm: Delta epsilon(434)(max) + 337, Delta epsilon(389)(max) - 186 (CHCl(3)), and Delta epsilon(431)(max) + 285, Delta epsilon(386)(max) - 177 (CH(3)OH). However, introduction of an amine into a CHCl(3) solution of 1 causes the Cotton effect signs to become inverted, e.g., after addition of NH(3), Delta epsilon(433)(max) - 345, Delta epsilon(389)(max) + 243, and after addition of ethylene diamine, Delta epsilon(435)(max) - 420, Delta epsilon(390)(max) + 299. The sign inversions imply inversion of molecular chirality of the bilirubin and the phenomenon appears to be general for amines, including alpha,omega-diamines. 1,8-Diaminooctane was found to be more effective than longer or shorter chain analogs in producing CD sign inversion.

  8. Impurity trapped excitons under high hydrostatic pressure

    NASA Astrophysics Data System (ADS)

    Grinberg, Marek

    2013-09-01

    Paper summarizes the results on pressure effect on energies of the 4fn → 4fn and 4fn-15d1 → 4fn transitions as well as influence of pressure on anomalous luminescence in Lnα+ doped oxides and fluorides. A model of impurity trapped exciton (ITE) was developed. Two types of ITE were considered. The first where a hole is localized at the Lnα+ ion (creation of Ln(α+1)+) and an electron is attracted by Coulomb potential at Rydberg-like states and the second where an electron captured at the Lnα+ ion (creation of Ln(α-1)+) and a hole is attracted by Coulomb potential at Rydberg-like states. Paper presents detailed analysis of nonlinear changes of energy of anomalous luminescence of BaxSr1-xF2:Eu2+ (x > 0.3) and LiBaF3:Eu2+, and relate them to ITE-4f65d1 states mixing.

  9. Benchmarking Calculations of Excitonic Couplings between Bacteriochlorophylls.

    PubMed

    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. PMID:26651217

  10. Singlet fission of hot excitons in π-conjugated polymers

    PubMed Central

    Zhai, Yaxin; Sheng, Chuanxiang; Vardeny, Z. Valy

    2015-01-01

    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≈2ET (=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>2ET, 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=Eg (≈2.25 eV). From this, we infer that intrachain SF that involves a triplet–triplet pair state, also known as the ‘dark’ 2Ag exciton, dominates the triplet photogeneration in PDA polymer as Eg>2ET. 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. PMID:25987576

  11. Intermolecular exciton-exciton annihilation in phospholipid vesicles doped with [Ru(bpy)2dppz]2+

    NASA Astrophysics Data System (ADS)

    De la Cadena, Alejandro; Pascher, Torbjörn; Davydova, Dar'ya; Akimov, Denis; Herrmann, Felix; Presselt, Martin; Wächtler, Maria; Dietzek, Benjamin

    2016-01-01

    The ultrafast photophysics of [Ru(bpy)2dppz]2+ (dppz = dipyrido[3,2-a:2‧,3‧-c]-phenazine) embedded into the walls of phospholipid vesicles has been studied by femtosecond time-resolved pump-probe spectroscopy. While [Ru(bpy)2dppz]2+ has been studied intensively with respect to its intramolecular charge transfer processes, which are associated with the well known light-switch effect, this study focuses on intermolecular energy transfer processes taking place upon dense packing of the complexes into a phospholipid membrane composed of dipalmitoyl-L-α-phosphatidylglycerol, which can be thought of as a simplistic model of a cellular membrane. The data indicate additional quenching of excited [Ru(bpy)2dppz]2+ upon increasing the pump-pulse intensity. Hence, the observed photophysics, which is assigned to the presence of intermolecular exciton-exciton annihilation at high pump-intensities, might be related to the ultrafast photophysics of [Ru(bpy)2dppz]2+ when used as a chromophore to stain cells, an effect that may be taken into account during the employment of novel cellular markers based on Ru polypyridine complexes.

  12. 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.

  13. 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.

  14. Dynamics of exciton formation and relaxation in photoexcited semiconductors

    NASA Astrophysics Data System (ADS)

    Janković, Veljko; Vukmirović, Nenad

    2015-12-01

    We investigate the dynamics of the exciton formation and relaxation on a picosecond time scale following a pulsed photoexcitation of a semiconductor. The study is conducted in the framework of the density matrix theory complemented with the dynamics controlled truncation scheme. We truncate the phonon branch of the resulting hierarchy of equations and propose the form of coupling among single-phonon-assisted and higher-order phonon-assisted density matrices so as to ensure the energy and particle-number conservation in a closed system. Time scales relevant for the exciton formation and relaxation processes are determined from numerical investigations performed on a one-dimensional model for the values of model parameters representative of a typical organic and inorganic semiconductor. The exciton dynamics is examined for different values of central frequency of the exciting field, temperature, and microscopic model parameters, such as the strengths of carrier-carrier and carrier-phonon couplings. We find that for typical organic semiconductor parameters, formation of bound excitons occurs on a several-hundred-femtosecond time scale, while their subsequent relaxation and equilibration take at least several picoseconds. These time scales are consistent with recent experimental studies of the exciton formation and relaxation in conjugated polymer-based materials.

  15. Inverse Funnel Effect of Excitons in Strained Black Phosphorus

    NASA Astrophysics Data System (ADS)

    San-Jose, Pablo; Parente, Vincenzo; Guinea, Francisco; Roldán, Rafael; Prada, Elsa

    2016-07-01

    We study the effects of strain on the properties and dynamics of Wannier excitons in monolayer (phosphorene) and few-layer black phosphorus (BP), a promising two-dimensional material for optoelectronic applications due to its high mobility, mechanical strength, and strain-tunable direct band gap. We compare the results to the case of molybdenum disulphide (MoS2 ) monolayers. We find that the so-called funnel effect, i.e., the possibility of controlling exciton motion by means of inhomogeneous strains, is much stronger in few-layer BP than in MoS2 monolayers and, crucially, is of opposite sign. Instead of excitons accumulating isotropically around regions of high tensile strain like in MoS2 , excitons in BP are pushed away from said regions. This inverse funnel effect is moreover highly anisotropic, with much larger funnel distances along the armchair crystallographic direction, leading to a directional focusing of exciton flow. A strong inverse funnel effect could enable simpler designs of funnel solar cells and offer new possibilities for the manipulation and harvesting of light.

  16. Hybrid quadrupole excitons and polaritons in cuprous oxide

    NASA Astrophysics Data System (ADS)

    Roslyak, Oleksiy

    In this thesis I consider novel type of materials such as hybrid organic/inorganic heteoro-structures and polystyrene micro-spheres/inorganic composites. The organic/inorganic compound is presented by DCM2:CA:PS/cuprous oxide material. Using "solid state solvent" mechanism I propose to bring the Frenkel exciton (FE) of the DCM2 into resonance with 1S quadrupole Wanier-Mott exciton (WE) in cuprous oxide. This two types of the excitons form new type of quadrupole-dipole hybrid exciton. This hybrid is characterized by long lifetime and big oscillator strength inherited from the organic FE. In the part I of the thesis I investigate the enhancement of the quadrupole properties generic to cuprous oxide exciton by means of such resonant hybridization. I consider enhancement of photo-thermal bi-stability and second harmonic generation. The second part is devoted to the problems of light-matter interaction in cuprous oxide crystals such as weak interaction with LA phonons and whispering gallery modes (WGM) in adjacent layer of polystyrene micro-spheres. While the first effect is likely to impeded BEC of the polaritons, the second mechanism provides necessary temporal coherence. It is possible by trapping the light part of the polariton into resonant WGM through big gradient of the evanescent tail which provides big lifetime of such evanescent polariton. Due to big gradient of the evanescent field it couples "naturally" to the quadrupole WE in cuprous oxide.

  17. Fundamental processes of exciton scattering at organic solar-cell interfaces: One-dimensional model calculation

    NASA Astrophysics Data System (ADS)

    Masugata, Yoshimitsu; Iizuka, Hideyuki; Sato, Kosuke; Nakayama, Takashi

    2016-08-01

    Fundamental processes of exciton scattering at organic solar-cell interfaces were studied using a one-dimensional tight-binding model and by performing a time-evolution simulation of electron–hole pair wave packets. We found the fundamental features of exciton scattering: the scattering promotes not only the dissociation of excitons and the generation of interface-bound (charge-transferred) excitons but also the transmission and reflection of excitons depending on the electron and hole interface offsets. In particular, the dissociation increases in a certain region of an interface offset, while the transmission shows resonances with higher-energy bound-exciton and interface bound-exciton states. We also studied the effects of carrier-transfer and potential modulations at the interface and the scattering of charged excitons, and we found trap dissociations where one of the carriers is trapped around the interface after the dissociation.

  18. Polaron conductivity mechanism in potassium acid phthalate crystal: AC-conductivity investigation

    NASA Astrophysics Data System (ADS)

    Filipič, Cene; Levstik, Iva; Levstik, Adrijan; Hadži, Dušan

    2016-08-01

    The complex dielectric constant, \\varepsilon *(ν ,T), of potassium acid phthalate monocrystal (KAP) was investigated over the broad frequency and temperature range. While the imaginary part of dielectric constant ε‧‧(ν) increases rapidly with increasing temperature in the studied temperature range, the real part of dielectric constant ε‧(ν) increases only at high temperatures; there is almost no change of ε‧(ν) below 200 K. Both values of ε‧ and ε‧‧ are frequency dependent; the values increase with decreasing frequencies. At temperatures below 450 K the ac electrical conductivity and dielectric constant follow simultaneously the universal dielectric response (UDR). The analysis of the temperature dependence of the UDR parameter s in terms of the theoretical model for small polarons revealed that this mechanism governs the charge transport in KAP crystal in the studied temperature range.

  19. Phonon-mediated interactions and polaron formation of slow-light polaritons in a BEC

    NASA Astrophysics Data System (ADS)

    Haug, Hanna-Lena; Fleischhauer, Michael

    2014-05-01

    We study the motion of dark-state polaritons (DSP) in a Bose-Einstein condensate. DSPs are formed in an atomic ensemble interacting in a Λ-type configuration with two light fields under conditions of electromagnetically induced transparency. In particular, we consider the ground-state atoms to form a BEC which can be well described by a macroscopic Gross-Pitaevskii wavefunction. Taking into account the interaction of pairs of ground-state atoms and between ground and spin-state atoms leads to the formation of polaronic quasi-particles consisting of DSPs and Bogoliubov phonons. In additon, the coupling to phonons results into a coupling between dark and bright-state polaritons as well as into phonon-mediated interactions between DSPs.

  20. Trimers, Molecules, and Polarons in Mass-Imbalanced Atomic Fermi Gases

    SciTech Connect

    Mathy, Charles J. M.; Parish, Meera M.; Huse, David A.

    2011-04-22

    We consider the ground state of a single ''spin-down'' impurity atom interacting attractively with a ''spin-up'' atomic Fermi gas. By constructing variational wave functions for polarons, molecules, and trimers, we perform a detailed study of the transitions between these dressed bound states as a function of mass ratio r=m{sub {up_arrow}}/m{sub {down_arrow}} and interaction strength. Crucially, we find that the presence of a Fermi sea enhances the stability of the p-wave trimer, which can be viewed as a Fulde-Ferrell-Larkin-Ovchinnikov molecule that has bound an additional majority atom. For sufficiently large r, we find that the transitions lie outside the region of phase separation of the imbalanced Fermi gas and should thus be observable in experiment, unlike the well-studied equal-mass case.