Science.gov

Sample records for impurity-bound small polarons

  1. Small polaron hopping transport along DNA molecules

    NASA Astrophysics Data System (ADS)

    Triberis, G. P.; Simserides, C.; Karavolas, V. C.

    2005-05-01

    We present a small polaron hopping model for interpreting the strong temperature (T) dependence of the electrical conductivity, σ, observed at high (h) temperatures along DNA molecules. The model takes into account the one-dimensional character of the system and the presence of disorder in the DNA double helix. Percolation-theoretical considerations lead to analytical expressions for the high temperature multiphonon-assisted small polaron hopping conductivity, the hopping distance and their temperature dependence. The experimental data for lambda phage DNA (λ-DNA) and poly(dA)-poly(dT) DNA follow nicely the theoretically predicted behaviour (lnσh~T-2/3). Moreover, our model leads to realistic values of the maximum hopping distances, supporting the idea of multiphonon-assisted hopping of small polarons between next nearest neighbours of the DNA molecular 'wire'. The low temperature case is also investigated.

  2. 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.

  3. 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

  4. Vacancies and small polarons in SrTiO3

    NASA Astrophysics Data System (ADS)

    Janotti, Anderson; Varley, Joel B.; Choi, Minseok; Van de Walle, Chris G.

    2014-08-01

    Using first-principles calculations we investigate the impact of intrinsic defects and small polarons on the electrical and optical properties of SrTiO3. We pay special attention to the seemingly contradictory role of oxygen vacancies as shallow donor and source of deep-level luminescence, as reported in the literature. We find that oxygen vacancies are double donors, and that one electron is easily ionized, explaining the shallow donor behavior. The second electron is trapped in the form of a small polaron, and this additional binding energy explains the behavior as a deep center that gives rise to blue luminescence. At low temperatures, holes become self-trapped, and recombination of free electrons with self-trapped holes gives rise to green luminescence. These results explain the intricate interplay between the observed green and blue luminescence in SrTiO3, and form a framework for interpreting similar phenomena in other complex oxides.

  5. Thermoelectric power of small polarons in magnetic semiconductors

    SciTech Connect

    Liu, N.H.; Emin, D.

    1984-09-15

    The thermoelectric power (Seebeck coefficient) ..cap alpha.. of a small polaron in both ferromagnetic and antiferromagnetic semiconductors and insulators is calculated for the first time. In particular, we obtain the contribution to the Seebeck coefficient arising from exchange interactions between the severely localized carrier (i.e., small polaron) of charge q and the spins of the host lattice. In essence, we study the heat transported along with a carrier. This heat, the Peltier heat, Pi, is related to the Seebeck coefficient by the Kelvin relation: Pi = qT..cap alpha.., where T is the temperature. The heat per carrier is simply the product of the temperature and the change of the entropy of the system when a small polaron is added to it. The magnetic contribution to the Seebeck coefficient is therefore directly related to the change of the magnetic entropy of the system upon introduction of a charge carrier. We explicitly treat the intrasite and intersite exchange interactions between a small polaron and the spins of a spin-1/2 system. These magnetic interactions produce two competing contributions to the Seebeck coefficient. First, adding the carrier tends to provide extra spin freedom (e.g., spin up or spin down of the carrier). This effect augments the entropy of the system, thereby producing a positive contribution to the Peltier heat. Second, however, the additional exchange between the carrier and the sites about it enhances the exchange binding among these sites. This generally reduces the energetically allowable spin configurations. The concomitant reduction of the system's entropy provides a negative contribution to the Peltier heat. At the highest of temperatures, when kT exceeds the intrasite exchange energy, the first effect dominates. Then, the Peltier heat is simply augmented by kT ln2.

  6. Unravelling Small-Polaron Transport in Metal Oxide Photoelectrodes.

    PubMed

    Rettie, Alexander J E; Chemelewski, William D; Emin, David; Mullins, C Buddie

    2016-02-01

    Transition-metal oxides are a promising class of semiconductors for the oxidation of water, a process that underpins both photoelectrochemical water splitting and carbon dioxide reduction. However, these materials are limited by very slow charge transport. This is because, unlike conventional semiconductors, material aspects of metal oxides favor the formation of slow-moving, self-trapped charge carriers: small polarons. In this Perspective, we seek to highlight the salient features of small-polaron transport in metal oxides, offer guidelines for their experimental characterization, and examine recent transport studies of two prototypical oxide photoanodes: tungsten-doped monoclinic bismuth vanadate (W:BiVO4) and titanium-doped hematite (Ti:α-Fe2O3). Analysis shows that conduction in both materials is well-described by the adiabatic small-polaron model, with electron drift mobility (distinct from the Hall mobility) values on the order of 10(-4) and 10(-2) cm(2) V(-1) s(-1), respectively. Future directions to build a full picture of charge transport in this family of materials are discussed. PMID:26758715

  7. Small polarons and point defects in barium cerate

    NASA Astrophysics Data System (ADS)

    Swift, Michael; Janotti, Anderson; Van de Walle, Chris G.

    2015-12-01

    Barium cerate (BaCeO3) is a well-known ionic conductor of both hydrogen and oxygen. In applications, it is frequently doped (for instance with Y) to increase stability and promote diffusion. However, the effects of doping and native defects are not fully understood. Computational studies have been stymied by the nature of the conduction band, which is made up of cerium 4 f states. These states present a challenge to ab initio techniques based on density functional theory within the standard approximations for exchange and correlation. Using a hybrid functional, we investigate the effects of hydrogen impurities and native defects on the electrical and optical properties of BaCeO3. We discuss the tendency of excess electrons or holes to localize in the form of small polarons. We also explore the interactions of polarons with hydrogen impurities and oxygen vacancies, and their impact on luminescence properties.

  8. Peltier heat of a small polaron in a magnetic semiconductor

    SciTech Connect

    Liu, N.H.; Emin, D.

    1985-04-15

    For the first time the heat transported with a small polaron in both antiferromagnetic and ferromagnetic semiconductors is calculated. This heat, the Peltier heat, ..pi.., is obtained from the change of the entropy of the total system upon introduction of a charge carrier. We explicitly consider both the intrasite and intersite exchange interactions between a small polaron and the interacting spins of a spin-1/2 magnet. There are two competing magnetic contributions to the Peltier heat. First, adding the carrier increases the spin entropy of the system. This provides a positive contribution to ..pi... Second, the exchange between the carrier and the sites about it enhances the exchange binding between these sites. This reduces the energetically allowable spin configurations and provides a negative contribution to ..pi... At extremely high temperatures when kT exceeds the intrasite exchange energy, the first effect dominates. Then ..pi.. is simply augmented by kT ln 2. However, well below the magnetic transition temperature the second effect dominates. In the experimentally accessible range between these limits both effects are comparable and sizable. The net magnetic contribution to the Peltier heat rises with temperature. Thus, a carrier's interactions with its magnetic environment produces a significant and distinctive contribution to its Peltier heat.

  9. Peltier heat of a small polaron in a magnetic semiconductor

    SciTech Connect

    Liu, N.L.H.; Emin, D.

    1984-01-01

    The heat transported with a small polaron in both antiferromagnetic and ferromagnetic semiconductors is calculated. This heat, the Peltier heat, ..pi.., is obtained from the change of the entropy of the total system upon introduction of a charge carrier. We explicitly consider both the intrasite and intersite exchange interactions between a small polaron and the interacting spins of a spin-1/2 magnet. There are two competing magnetic contributions to the Peltier heat. First, adding the carrier increases the spin entropy of the system. This provides a positive contribution to ..pi... Second, the exchange between the carrier and the sites about it enhances the exchange binding between these sites. This reduces the energetically allowable spin configurations and provides a negative contribution to ..pi... At extremely high temperature when kT exceeds the intrasite exchange energy, the first effect dominates. Then ..pi.. is simply augmented by kTln2. However, well below the magnetic transition temperature the second effect dominates. In the experimentally accessible range between these limits both effects are comparable and sizable. The net magnetic contribution to the Peltier heat rises with temperature. Thus, a carrier's interactions with its magnetic environment produces a significant and distinctive contribution to its Peltier heat.

  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. 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.

  12. High temperature electrical conductivity due to small polaron hopping motion in DNA molecules

    NASA Astrophysics Data System (ADS)

    Triberis, G. P.; Karavolas, V. C.; Simserides, C. D.

    2005-01-01

    We present a small polaron hopping model to interpret the high-temperature electrical conductivity measured along the DNA molecules. The model takes into account the one-dimensional character of the system and the presence of disorder in the DNA double helix. The experimental data for the lambda phage DNA (λ-DNA) and the poly(dA)-poly(dT) DNA follow nicely the theoretically predicted behavior leading to realistic values of the maximum hopping distances supporting the idea of multiphonon-assisted hopping of small polarons between next nearest neighbors of the DNA molecular "wire".

  13. 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.

  14. 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.

  15. Point defects, impurities, and small hole polarons in GdTiO3

    NASA Astrophysics Data System (ADS)

    Bjaalie, L.; Janotti, A.; Krishnaswamy, K.; Van de Walle, C. G.

    2016-03-01

    The electronic structure of native defects and impurities in GdTiO3, a rare-earth titanate Mott insulator, is studied using density functional theory with a hybrid functional. Among native defects, the cation vacancies have the lowest formation energies in oxygen-rich conditions and oxygen vacancies have the lowest formation energy in oxygen-poor conditions. Among the impurities, SrGd,Hi, and CO have low formation energies. A common feature of the native defects and impurities is that they lead to the formation of small hole polarons, which explains the frequent observation of p -type hopping conductivity in the rare-earth titanates. These small hole polarons also lead to optical absorption and act as electron traps in devices.

  16. High-density Two-Dimensional Small Polaron Gas in a Delta-Doped Mott Insulator

    PubMed Central

    Ouellette, Daniel G.; Moetakef, Pouya; Cain, Tyler A.; Zhang, Jack Y.; Stemmer, Susanne; Emin, David; Allen, S. James

    2013-01-01

    Heterointerfaces in complex oxide systems open new arenas in which to test models of strongly correlated material, explore the role of dimensionality in metal-insulator-transitions (MITs) and small polaron formation. Close to the quantum critical point Mott MITs depend on band filling controlled by random disordered substitutional doping. Delta-doped Mott insulators are potentially free of random disorder and introduce a new arena in which to explore the effect of electron correlations and dimensionality. Epitaxial films of the prototypical Mott insulator GdTiO3 are delta-doped by substituting a single (GdO)+1 plane with a monolayer of charge neutral SrO to produce a two-dimensional system with high planar doping density. Unlike metallic SrTiO3 quantum wells in GdTiO3 the single SrO delta-doped layer exhibits thermally activated DC and optical conductivity that agree in a quantitative manner with predictions of small polaron transport but with an extremely high two-dimensional density of polarons, ~7 × 1014 cm−2. PMID:24257578

  17. 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.

  18. Anisotropic small-polaron hopping in W:BiVO4 single crystals

    NASA Astrophysics Data System (ADS)

    Rettie, Alexander J. E.; Chemelewski, William D.; Lindemuth, Jeffrey; McCloy, John S.; Marshall, Luke G.; Zhou, Jianshi; Emin, David; Mullins, C. Buddie

    2015-01-01

    DC electrical conductivity, Seebeck and Hall coefficients are measured between 300 and 450 K on single crystals of monoclinic bismuth vanadate that are doped n-type with 0.3% tungsten donors (W:BiVO4). Strongly activated small-polaron hopping is implied by the activation energies of the Arrhenius conductivities (about 300 meV) greatly exceeding the energies characterizing the falls of the Seebeck coefficients' magnitudes with increasing temperature (about 50 meV). Small-polaron hopping is further evidenced by the measured Hall mobility in the ab-plane (10-1 cm2 V-1 s-1 at 300 K) being larger and much less strongly activated than the deduced drift mobility (about 5 × 10-5 cm2 V-1 s-1 at 300 K). The conductivity and n-type Seebeck coefficient is found to be anisotropic with the conductivity larger and the Seebeck coefficient's magnitude smaller and less temperature dependent for motion within the ab-plane than that in the c-direction. These anisotropies are addressed by considering highly anisotropic next-nearest-neighbor (≈5 Å) transfers in addition to the somewhat shorter (≈4 Å), nearly isotropic nearest-neighbor transfers.

  19. 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.

  20. 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.

  1. Appearance of small polaron hopping conduction in iron modified cobalt lithium bismuth borate glasses

    NASA Astrophysics Data System (ADS)

    Dahiya, M. S.; Khasa, S.; Yadav, Arti; Agarwal, A.

    2016-05-01

    Lithium bismuth borate glasses containing different amounts of cobalt and iron oxides having chemical composition xFe2O3•(20-x)CoO•30Li2O•10Bi2O3•40B2O3 (x = 0, 5, 10, 15 and 20 mol% abbreviated as CFLBB1-5 respectively) prepared via melt quench technique have been investigated for their dc electrical conductivity. The amorphous nature of prepared glasses has been confirmed through X-ray diffraction measurements. The dc electrical conductivity has been analyzed by applying Mott's small polaron hopping model. Activation energies corresponding to lower and higher temperature region have been evaluated. The iron ion concentration (N), mean spacing between iron ions (R) and polaron radius (Rp) has been evaluated using the values of phonon radius (Rph) and Debye temperature (θD). The glass sample without iron (CFLBB1) shows ionic conductivity but the incorporation of iron in the glass matrix results in the appearance of electronic conductivity.

  2. Point defects, impurities, and small hole polarons in GdTiO3

    NASA Astrophysics Data System (ADS)

    Bjaalie, Lars; Janotti, Anderson; Krishnaswamy, Karthik; van de Walle, Chris G.

    GdTiO3(GTO) has become the focus of great interest because of its use in complex-oxide heterostructures that display two-dimensional electron gases with unprecedented high densities. GTO is a Mott insulator, with a band gap arising within the partially filled Ti 3 d band due to strong electron-electron interactions. GTO often displays hole conductivity, likely attributed to defects or impurities, yet the cause of this unintentional conductivity has not yet been explored. We therefore used density functional theory with a hybrid functional to study their electronic structure. Among native defects, the cation vacancies have the lowest formation energies in oxygen-rich conditions, and oxygen vacancies have the lowest formation energy in oxygen-poor conditions. Among the impurities, rGd, Hi and CO have the lowest formation energies. The defects and impurities are intrinsically stable only in a single ``natural'' charge state, to which various numbers of hole polarons can be bound, which explains the frequent observation of p-type hopping conductivity in the rare-earth titanates. These small hole polarons also lead to optical absorption and act as electron traps in devices. Work supported by NSF and by the LEAST Center.

  3. Formation of small polarons in Li2O2 and implications for Li-air batteries

    NASA Astrophysics Data System (ADS)

    Kang, Joongoo; Jung, Yoon-Seok; Wei, Su-Huai; Dillon, Anne

    2012-02-01

    Lithium-air batteries (LABs) have recently been revitalized as a promising electrical energy storage system due to their exceptionally high theoretical energy density. However, its usage is limited by poor rate capability and large polarization in the cell voltage due primarily to the formation of Li2O2 in the air cathode. Here, using hybrid density functional theory, we found that the formation of small polarons in Li2O2 is the origin that limits the electron transport in Li2O2. Consequently, the low electron mobility contributes to the hysteresis in cell voltage and limits the power density of the LABs. We suggest that similar behavior should exist in other peroxides, and p-type doping in Li2O2 could significantly improve the performance of LABs at high current densities.

  4. Donor defects and small polarons on the TiO2(110) surface

    NASA Astrophysics Data System (ADS)

    Moses, P. G.; Janotti, A.; Franchini, C.; Kresse, G.; Van de Walle, C. G.

    2016-05-01

    The role of defects in the chemical activity of the rutile TiO2(110) surface remains a rich topic of research, despite the rutile (110) being one of the most studied surfaces of transition-metal oxides. Here, we present results from hybrid functional calculations that reconcile apparently disparate views on the impact of donor defects, such as oxygen vacancies and hydrogen impurities, on the electronic structure of the (110) rutile surface. We find that the bridging oxygen vacancy and adsorbed or substitutional hydrogen are actually shallow donors, which do not induce gap states. The excess electrons from these donor centers tend to localize in the form of small polarons, which are the factual cause of the deep states ˜1 eV below the conduction band, often observed in photoelectron spectroscopy measurements. Our results offer a new framework for understanding the surface electronic structure of TiO2 and related oxides.

  5. Delayed luminescence from collagen as arising from soliton and small polaron states

    NASA Astrophysics Data System (ADS)

    Scordino, Agata; Grasso, Rosaria; Gulino, Marisa; Lanzanà, Luca; Musumeci, Francesco; Privitera, Giuseppe; Tedesco, Maurizio; Triglia, Antonio; Brizhik, Larissa

    With the aim to give more hints to a theoretical model that describes the phenomenon of delayed luminescence (DL) from biological systems as due to the collective electron states that are excited in macromolecular structures by external illumination, a spectral characterization of DL from bovine Achilles' tendons sample at different hydration states has been performed. Tendons are mainly composed by Type I collagen macromolecules which form a one-dimensional system with the long-range order and capability of self-organization, so favoring the existence of such collective excitations. Modeling the crystal structure of collagen as a one-dimensional chain whose unit cell is formed by a tripeptide, the ground state of the corresponding Hamitonian has been evaluated by a variational approach. The change in DL from bovine Achilles' tendons, depending on the water content of the sample, has been correlated to the change in the ground state of such one-dimensional lattice from a soliton state, for samples close to native, to a small polaron state, for samples that are much more dry.

  6. Electron small polarons and their mobility in iron (oxyhydr)oxide nanoparticles

    SciTech Connect

    Katz, Jordan E.; Zhang, Xiaoyi; Attenkofer, Klaus; Chapman, Karena W.; Frandsen, Cathrine; Zarzycki, Piotr P.; Rosso, Kevin M.; Falcone, Roger; Waychunas, Glenn; Gilbert, Benjamin

    2012-09-07

    Redox-active transition metal (TM) oxides, hydroxide and oxyhydroxides semiconductors typically posses wide p-d charge-transfer band gaps and exhibit poor charge carrier mobility. Nevertheless, there is increasing evidence that electron mobility within TM (oxyhydr)oxides is a crucial feature of their redox reactivity, affecting the rates of interfacial reactions, outcomes of redox-driven phase transformations and enabling charge transfer between reactions occurring at widely-separated surface sites 1,2. In order to determine the links between crystal structure and charge transport efficiency on solid-phase redox reactivity we have applied a pump-probe method to observe directly the fate of electrons introduced into ferric iron (oxyhydr)oxide nanoparticles via ultrafast interfacial electron transfer3. Time-resolved X-ray spectroscopy observes the formation of reduced and structurally distorted metal sites consistent with small polarons. By tracking the lifetime of the reduced metal states, rate constants for thermally-activated cation-to-cation electron hopping in the solid can be measured with subnanosecond accuracy. Comparisons between different phases revealed that short-range structural topology, not long-range order, dominates the electron-hopping rate, and shed new insight into the structure and properties of the naturally-formed nanomaterial, ferrihydrite4. Lattice Monte Carlo simulations revealed that, on timescales relevant to solid-phase reactions, surface charge plays a commanding role in biasing electron conduction trajectories.

  7. A small polaron hopping model for multiphonon-assisted transport along DNA molecules, in the presence of disorder

    NASA Astrophysics Data System (ADS)

    Triberis, Georgios; Simserides, Constantinos; Karavolas, Vasileios

    2006-05-01

    We discuss a small polaron hopping model, in order to explain the intense temperature ( T) dependence of the electrical conductivity (σ) observed at high temperatures along the DNA molecules. The model takes into account the one-dimensional character of the system as well as the presence of disorder in the DNA double helix. Theoretical considerations based on percolation lead to analytical expressions for the high temperature multiphonon-assisted small polaron hopping conductivity, the maximum hopping distance and their temperature dependence. For example, experimental data for the λ-phage DNA, the poly(dA)-poly(dT) DNA, and the native wet-spun calf thymus Li-DNA, follow nicely the theoretically predicted behavior, lnσh∝T, over wide high- T ranges. In contrast to some previously presented theoretical suggestions, our model leads to realistic values for the maximum hopping distances, supporting the idea of multiphonon-assisted hopping of small polarons between next nearest neighbors of the DNA molecular “wire”. We also examine the low temperature case.

  8. Transmon-based simulator of nonlocal electron-phonon coupling: A platform for observing sharp small-polaron transitions

    NASA Astrophysics Data System (ADS)

    Stojanović, Vladimir M.; Vanević, Mihajlo; Demler, Eugene; Tian, Lin

    2014-04-01

    We propose an analog superconducting quantum simulator for a one-dimensional model featuring momentum-dependent (nonlocal) electron-phonon couplings of Su-Schrieffer-Heeger and "breathing-mode" types. Because its corresponding coupling vertex function depends on both the electron and phonon quasimomenta, this model does not belong to the realm of validity of the Gerlach-Löwen theorem that rules out any nonanalyticities in single-particle properties. The superconducting circuit behind the proposed simulator entails an array of transmon qubits and microwave resonators. By applying microwave driving fields to the qubits, a small-polaron Bloch state with an arbitrary quasimomentum can be prepared in this system within times several orders of magnitude shorter than the typical qubit decoherence times. We demonstrate that—by varying the externally tunable parameters—one can readily reach the critical coupling strength required for observing the sharp transition from a nondegenerate (single-particle) ground state corresponding to zero quasimomentum (Kgs=0) to a twofold-degenerate small-polaron ground state at nonzero quasimomenta Kgs and -Kgs. Through exact numerical diagonalization of our effective Hamiltonian, we show how this nonanalyticity is reflected in the relevant single-particle properties (ground-state energy, quasiparticle residue, average number of phonons). We also show that the proposed setup provides an ideal testbed for studying the nonequilibrium dynamics of small-polaron formation in the presence of strongly momentum-dependent electron-phonon interactions.

  9. Optical absorption and small-polaron hopping in oxygen deficient and lithium-ion-intercalated amorphous titanium oxide films

    NASA Astrophysics Data System (ADS)

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

    2016-01-01

    Optical absorption in oxygen-deficient and Li+-ion inserted titanium oxide films was studied in the framework of small-polaron hopping. Non-stoichiometric TiOy films with 1.68 ≤ y ≤ 2.00 were deposited by reactive DC magnetron sputtering and were subjected to electrochemical intercalation of Li+-ions and charge-balancing electrons to obtain LixTiOy films with 0.12 ≤ x ≤ 0.34. Dispersion analysis was applied to calculate the complex dielectric function ɛ(ℏω) ≡ ɛ1(ℏω) + i ɛ2(ℏω) from numerical inversion of optical transmittance and reflectance spectra; a superposition of Tauc-Lorentz and Lorentz oscillator models was used for this purpose. Data on ɛ2(ℏω) were employed to calculate the optical conductivity and fit this property to a small-polaron model for disordered systems with strong electron-phonon interaction and involving transitions near the Fermi level. The introduction of oxygen vacancies and/or Li+ insertion yielded band gap widening by ˜0.20-0.35 eV, and both processes induced similar low-energy optical absorption. The small-polaron-based analysis indicated increases in the Fermi level by ˜0.15-0.3 eV for sub-stoichiometric and/or Li+-inserted films. This suggests the existence of polaronic Ti3+ states in the lower part of the conduction band arising from transfer of electrons from oxygen vacancies and/or inserted Li+ species. The present article is a sequel to an earlier paper on oxygen-deficient and/or Li+-inserted amorphous WOy thin films and forms part of a comprehensive investigation of optical absorption in amorphous transition metal oxides with different valence states of the metallic ions.

  10. Anisotropic spin dephasing of impurity-bound electron spins in ZnO

    SciTech Connect

    Lee, Jieun; Sih, Vanessa; Venugopal, Aneesh

    2015-01-05

    We investigate the electron spin dynamics of n-type c-axis oriented bulk zinc oxide (ZnO) by using time-resolved Kerr rotation and resonant spin amplification measurements. Calculating resonant spin amplification using an anisotropic spin dephasing model reveals that there are two species involved in the spin dynamics, which we attribute to conduction and impurity-bound electron spins, respectively. We find that the impurity-bound electron spin dephasing mechanism is strongly anisotropic due to anisotropic exchange interactions. The identification of the two spin species and their dephasing mechanisms is further supported by the temperature, power, and wavelength dependence of the spin coherence measurements.

  11. Implications of the Formation of Small Polarons in Li2O2 for Li-Air Batteries

    SciTech Connect

    Kang, J.; Jung, Y. S.; Wei, S. H.; Dillon, A. C.

    2012-01-15

    Lithium-air batteries (LABs) are an intriguing next-generation technology due to their high theoretical energy density of {approx}11 kWh/kg. However, LABs are hindered by both poor rate capability and significant polarization in cell voltage, primarily due to the formation of Li{sub 2}O{sub 2} in the air cathode. Here, by employing hybrid density functional theory, we show that the formation of small polarons in Li{sub 2}O{sub 2} limits electron transport. Consequently, the low electron mobility {mu} = 10{sup -10}-10{sup -9} cm{sup 2}/V s contributes to both the poor rate capability and the polarization that limit the LAB power and energy densities. The self-trapping of electrons in the small polarons arises from the molecular nature of the conduction band states of Li{sub 2}O{sub 2} and the strong spin polarization of the O 2p state. Our understanding of the polaronic electron transport in Li{sub 2}O{sub 2} suggests that designing alternative carrier conduction paths for the cathode reaction could significantly improve the performance of LABs at high current densities.

  12. Implications of the formation of small polarons in Li2O2 for Li-air batteries

    NASA Astrophysics Data System (ADS)

    Kang, Joongoo; Jung, Yoon Seok; Wei, Su-Huai; Dillon, Anne C.

    2012-01-01

    Lithium-air batteries (LABs) are an intriguing next-generation technology due to their high theoretical energy density of ˜11 kWh/kg. However, LABs are hindered by both poor rate capability and significant polarization in cell voltage, primarily due to the formation of Li2O2 in the air cathode. Here, by employing hybrid density functional theory, we show that the formation of small polarons in Li2O2 limits electron transport. Consequently, the low electron mobility μ = 10-10-10-9 cm2/V s contributes to both the poor rate capability and the polarization that limit the LAB power and energy densities. The self-trapping of electrons in the small polarons arises from the molecular nature of the conduction band states of Li2O2 and the strong spin polarization of the O 2p state. Our understanding of the polaronic electron transport in Li2O2 suggests that designing alternative carrier conduction paths for the cathode reaction could significantly improve the performance of LABs at high current densities.

  13. Transmon-based simulator of nonlocal electron-phonon coupling: a platform for observing sharp small-polaron transitions

    NASA Astrophysics Data System (ADS)

    Stojanovic, Vladimir; Demler, Eugene; Vanevic, Mihajlo; Tian, Lin

    2014-03-01

    We propose an analog simulator for a one-dimensional model with momentum-dependent (nonlocal) electron-phonon couplings of Su-Schrieffer-Heeger and ``breathing-mode'' types. The superconducting circuit behind this simulator entails an array of transmon qubits and microwave resonators. Using a microwave-driving based protocol, small-polaron Bloch states with arbitrary quasimomentum can be prepared in this system within times several orders of magnitude shorter than the qubit decoherence time. We show that - by varying the circuit parameters - one can readily reach the critical coupling strength for observing the sharp transition from a nondegenerate single-particle ground state at zero quasimomentum (Kgs = 0) to a twofold degenerate small-polaron ground state corresponding to equal and opposite (nonzero) quasimomenta Kgs and -Kgs . Through exact diagonalization of our effective model, we show how this nonanalyticity is reflected in the relevant single-particle properties (ground-state energy, quasiparticle residue, average number of phonons). Our work paves the way for understanding the physical implications of strongly momentum-dependent electron-phonon interactions. Supported by the SNSF.

  14. Small hole polaron in CdTe: Cd-vacancy revisited

    PubMed Central

    Shepidchenko, A.; Sanyal, B.; Klintenberg, M.; Mirbt, S.

    2015-01-01

    The characteristics of electronic states of Cd-vacancies in CdTe, an important semiconductor for various technological applications, are under debate both from theoretical and experimental points of view. Experimentally, the Cd-vacancy in its negative charge state is found to have C3v symmetry and a (−1/−2) transition level at 0.4 eV. Our first principles density functional calculations with hybrid functionals confirm for the first time these experimental findings. Additionally, we find that the C3v symmetry and the position of the (−1/−2) transition level are caused by the formation of a hole polaron localised at an anionic site around the vacancy. PMID:26411338

  15. Hole polaron of small radius in assemblies of hydrated mono-protonated meso-tetraphenylporphine dimers at 77 K

    NASA Astrophysics Data System (ADS)

    Udal'tsov, Alexander V.

    2015-11-01

    Polaron theory is often used for the study of electrons and holes mobility in semiconductors when longitudinal optical (LO) phonons are generated upon the charge carriers moving. The polaron theory was applied to explain long-wavelength absorptions observed nearby Soret band in the electronic spectra of assemblies of mono-protonated meso-tetraphenylporphine dimer (TPP2H+) that are interpreted as LO-phonons originated due to proton movement. The energy of hole polaron is found to be 1.50 eV at 77 K. Energy of Franck-Condon transitions of LO-phonons generated by hole polaron moving through water confined in the assemblies with distortions of O-H bonds is 0.2653 eV (2138 cm-1). A broad band around 2127 cm-1 corresponding the same energy of O-H bonds vibrations is observed in IR spectra of the assemblies consisting of water and mainly of TPP2H+ species in the solid state indicating the presence of similar distortions of the hydrogen bonds. The radius of protonic sphere of 0.202 Å, which was estimated as a polaron quasiparticle moving through the confined water at 77 K, is found in agreement with earlier evaluated one of 0.265 Å that was obtained for proton diffusion at 298 K in similar assemblies.

  16. Infrared optical properties of α-alumina with the approach to melting: γ-like tetrahedral structure and small polaron conduction

    SciTech Connect

    Brun, J. F.; Campo, L. del; De Sousa Meneses, D.; Echegut, P.

    2013-12-14

    The normal spectral emittance of α-Al{sub 2}O{sub 3} single crystal has been measured from room temperature up to the liquid state and from 20 cm{sup −1} up to 10 000 cm{sup −1}, in two polarization configurations. The spectra were fitted with a semi-quantum dielectric function model. AlO{sub 4} structure units are revealed within the phonon spectral range more than a hundred degrees below the melting point when heating from the solid state. In parallel, the anomalous increase of emittance observed within the transparency spectral range with the approach to melting appears strongly correlated. Implications on the electronic structure are discussed: the existence of small polaron conduction is suggested which has never been mentioned before.

  17. Small polarons and magnetic antiphase boundaries in Ca2-xNaxCuO2Cl2 (x=0.06,0.12) : Origin of striped phases in cuprates

    NASA Astrophysics Data System (ADS)

    Patterson, C. H.

    2008-03-01

    We report hybrid density functional theory calculations on hole doped Ca2-xNaxCuO2Cl2 performed in 4×4 , 42×42 , and 8×2 supercells with hole concentrations x=0.0625 and x=0.125 . Holes at the lower concentration form small polarons, in which the hole is mainly localized on four oxygen ions surrounding one copper ion. The polaron is a spin one-half ferromagnetic polaron (Cu5O4) , in which the moment on the central copper ion is parallel to those on the four neighboring copper ions and the moment on the oxygen ions is opposed to that on the copper ions. This is therefore an Emery-Reiter spin polaron rather than a Zhang-Rice singlet. At the higher hole concentration (x=0.125) , many cuprates form stripes. Hybrid density functional theory calculations on linear chains of spin polarons separated by 4a0 show a group of bands localized mainly on the stripe. Spins on neighboring copper ions in the stripe are parallel and so the stripe forms a magnetic antiphase boundary between antiferromagnetically ordered blocks of copper spins. Stripes of this kind, which run in one direction only, may explain recent scanning tunneling microscopy data from Ca2-xNaxCuO2Cl2 by Kohsaka [Science 315, 1380 (2007)]. We also consider an ordered spin polaron phase where magnetic antiphase boundaries intersect at right angles. In this case, sets of four copper ions in squares at stripe intersections have parallel spins. This phase may be the 4×4 checkerboard pattern reported by Hanaguri [Nature (London) 430, 1001 (2004)].

  18. 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.

  19. 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.

  20. Localization, lattice distortion, charge transition levels, and magnetism of small-polaronic hole- and electron-states in wide-gap semiconductors

    NASA Astrophysics Data System (ADS)

    Lany, Stephan

    2010-03-01

    The formation of a small polaron, i.e. of a localized (electron or hole) quasi-particle state that is stabilized by a lattice distortion, is a problem in solid state physics that has eluded a quantitative description by first principles Hamiltonians for a long time. Specifically, conventional density functional theory calculations typically predict a much too delocalized state and usually fail to correctly predict the lattice distortions of localized hole-states in semiconductors and insulators. While this problem has been studied in detail for some prototypical cases like the Al impurity in SiO2, it has at the same time precluded an extensive theoretical literature on the phenomenology of systems with localized hole states, despite the potentially dramatic effect of hole localization on such timely research topics as p-type doping of oxides or that of diluted magnetic semiconductors. Indeed, many predictions for hole-introducing defects and impurities that were based on local density approximations have led to a qualitatively wrong physical picture about the lattice distortion, the energies of the hole-bearing acceptor levels in the gap, and about ferro-magnetic interactions between defects. In order to stabilize the polaronic localized states in the gap, we define a parameterized hole- (or electron-) state potential which increases the energy splitting between occupied and unoccupied orbitals, where we further require that a fundamental physical condition is satisfied, i.e., the piecewise linearity of the energy as a function of the occupation number. This requirement takes the form of a generalized Koopmans conditions, which uniquely determines the one free parameter of the hole- (electron-) state potential. Applying this method to the anion-p orbitals within the II-VI series of ZnO, ZnS, ZnSe, and ZnTe, we demonstrate electronic correlation effects remove the partial band occupation and the metallic band-structure character that is predicted by local density

  1. Effect of epitaxial strain on small-polaron hopping conduction in Pr{sub 0.7}(Ca{sub 0.6}Sr{sub 0.4}){sub 0.3}MnO{sub 3} thin films

    SciTech Connect

    Wang, Jing Hu, Feng-xia; Zhao, Ying-ying; Liu, Yao; Wu, Rong-rong; Sun, Ji-rong; Shen, Bao-gen

    2015-03-09

    We investigated the epitaxial strain effect on the small-polaron hopping conduction properties in Pr{sub 0.7}(Ca,Sr){sub 0.3}MnO{sub 3} (PCSMO) films. An increase in the carrier localization, as evidenced by the enhancement of the small-polaron activation energy E{sub A} in the high temperature region, was obtained by increasing the epitaxial lattice strain in either the tensile or compressive strained film. Furthermore, it was found that the magnitude of E{sub A}, and thus the carrier localization, strongly depends on the sign of the lattice strain, which explains the diverse percolative transport behaviors in PCSMO films with different types of strains. Meanwhile, similar dependencies on the strain of the films were also obtained for the electron-phonon interaction, characterized by the calculated small-polaron coupling constant. Our results reveal that the type of lattice strain plays a crucial role in determining the degree of localization of charge carriers and the electron-phonon coupling strength, which is important for understanding the lattice strain-induced various novel properties related to phase separation and percolation behaviors.

  2. Impurity effects on polaron-exciton formation in conjugated polymers

    SciTech Connect

    Ribeiro, Luiz Antonio Ferreira da Cunha, Wiliam; Neto de Oliveira, Pedro Henrique; Gargano, Ricardo; Magela e Silva, Geraldo

    2013-11-07

    Combining the one-dimensional tight-binding Su-Schrieffer-Heeger model and the extended Hubbard model, the collision of two oppositely charged polarons is investigated under the influence of impurity effects using a non-adiabatic evolution method. Results show that electron-electron interactions have direct influence on the charge distribution coupled to the polaron-exciton lattice defect. Additionally, the presence of an impurity in the collisional process reduces the critical electric field for the polaron-exciton formation. In the small electric field regime, the impurity effects open three channels and are of fundamental importance to favor the polaron-exciton creation. The results indicate that the scattering between polarons in the presence of impurities can throw a new light on the description of electroluminescence in conjugated polymer systems.

  3. Dielectric properties and study of AC electrical conduction mechanisms by non-overlapping small polaron tunneling model in Bis(4-acetylanilinium) tetrachlorocuprate(II) compound

    NASA Astrophysics Data System (ADS)

    Abkari, A.; Chaabane, I.; Guidara, K.

    2016-09-01

    In the present work, the synthesis and characterization of the Bis(4-acetylanilinium) tetrachlorocuprate(II) compound are presented. The structure of this compound is analyzed by X-ray diffraction which confirms the formation of single phase and is in good agreement the literature. Indeed, the Thermo gravimetric Analysis (TGA) shows that the decomposition of the compound is observed in the range of 420-520 K. However, the differential thermal analysis (DTA) indicates the presence of a phase transition at T=363 k. Furthermore, the dielectric properties and AC conductivity were studied over a temperature range (338-413 K) and frequency range (200 Hz-5 MHz) using complex impedance spectroscopy. Dielectric measurements confirmed such thermal analyses by exhibiting the presence of an anomaly in the temperature range of 358-373 K. The complex impedance plots are analyzed by an electrical equivalent circuit consisting of resistance, constant phase element (CPE) and capacitance. The activation energy values of two distinct regions are obtained from log σT vs 1000/T plot and are found to be E=1.27 eV (T<363 K) and E=1.09 eV (363 Ksmall polaron tunneling (NSPT) model is the most applicable conduction mechanism in the title compound. Complex impedance spectra of [C8H10NO]2CuCl4 at different temperatures.

  4. Two-Dimensional Polaronic Behavior in the Binary Oxides m-HfO2 and m-ZrO2

    SciTech Connect

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

    2012-03-14

    We demonstrate that the three-dimensional (3D) binary monoclinic oxides HfO2 and ZrO2 exhibit quasi-2D polaron localization and conductivity, which results from a small difference in the coordination of two oxygen sublattices in these materials. The transition between a 2D large polaron into a zerodimensional small polaron state requires overcoming a small energetic barrier. These results demonstrate how a small asymmetry in the lattice structure can determine the qualitative character of polaron localization and significantly broaden the realm of quasi-2D polaron systems.

  5. Two-Dimensional Polaronic Behavior in the Binary Oxides m-HfO2 and m-ZrO2

    SciTech Connect

    McKenna, K. P.; Wolf, M. J.; Shluger, A. L.; Lany, S.; Zunger, A.

    2012-03-16

    We demonstrate that the three-dimensional (3D) binary monoclinic oxides HfO{sub 2} and ZrO{sub 2} 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.

  6. 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

  7. Spontaneous polaron transport in biopolymers

    NASA Astrophysics Data System (ADS)

    Chakrabarti, B.; Piette, B. M. A. G.; Zakrzewski, W. J.

    2012-02-01

    Polarons, introduced by Davydov to explain energy transport in α-helices, correspond to electrons localised on a few lattice sites because of their interaction with phonons. While the static polaron field configurations have been extensively studied, their displacement is more difficult to explain. In this paper we show that, when the next-to-nearest-neighbour interactions are included, for physical values of the parameters, polarons can spontaneously move, at T=0, on bent chains that exhibit a positive gradient in their curvature. At room temperature polarons perform a random walk but a curvature gradient can induce a non-zero average speed similar to the one observed at zero temperature. We also show that, at zero temperature, a polaron bounces on sharply kinked junctions. We interpret these results in the light of the energy transport by transmembrane proteins.

  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. Bound polarons in semiconductor nanostructures

    NASA Astrophysics Data System (ADS)

    Woggon, U.; Miller, D.; Kalina, F.; Gerlach, B.; Kayser, D.; Leonardi, K.; Hommel, D.

    2003-01-01

    Bound polarons are discrete, confined electronic states, spatially localized due to a local potential V(r) but sharing a common phonon state of the surrounding crystal. We study the energy states of polarons bound in a potential and determine the local optical absorption spectrum up to first-order time-dependent perturbation theory with respect to the electron-photon interaction. The model is applied to describe the optical properties of submonolayer CdSe insertions epitaxially grown between ZnSe layers. As a typical signature of bound polarons we found excited-state energies equidistantly separated by the LO phonon energy and with optical transition probabilities determined by the anisotropies in V(r).

  11. Some approaches to polaron theory

    NASA Astrophysics Data System (ADS)

    Bogolubov, N. N.; Bogolubov, N. N.

    1985-11-01

    Here, in our approximation of polaron theory, we examine the importance of introducing the T product, which turn out to be a very convenient theoretical approach for the calculation of thermodynamical averages. We focus attention on the investigation of the so-called linear polaron Hamiltonian and present in detail the calculation of the correlation function, spectral function, and Green function for such a linear system. It is shown that the linear polaron Hamiltonian provides an exactly solvable model of our system, and the result obtained with this approach holds true for an arbitrary coupling constant which describes the strength of interaction between the electron and the lattice vibrations. Then, with the help of a variational technique, we show the possibility of reducing the real polaron Hamiltonian to a socalled trial or approximate linear model Hamiltonian. We also consider the exact calculation of free energy with a special technique that reduces calculations with the help of the T product, which, in our opinion, works much better and is easier than other analogous considerations, for example, the path-integral or Feynman-integral method.(1,2) Here we furthermore recall our own work,(4) where it was shown that the results of Refs. 7 and 8 concerning the impedance calculation in the polaron model may be obtained directly without the use of the path-integral method. The study of the polaron system's thermodynamics is carried out by us in the framework of the functional method. A calculation of the free energy and the momentum distribution function is proposed. Note also that the polaron systems with strong coupling(9) proved to be useful in different quantum field models in connection with the construction of dynamical models of composite particles. A rigorous solution of the special strong-coupling polaron problem, describing the interaction of a nonrelativistic particle with a quantum field, was given by Bogolubov.(3) The works of Tavkhelidze, Fedyanin

  12. Bloch oscillations of bosonic lattice polarons

    NASA Astrophysics Data System (ADS)

    Grusdt, F.; Shashi, A.; Abanin, D.; Demler, E.

    2014-12-01

    We consider a single-impurity atom confined to an optical lattice and immersed in a homogeneous Bose-Einstein condensate (BEC). Interaction of the impurity with the phonon modes of the BEC leads to the formation of a stable quasiparticle, the polaron. We use a variational mean-field approach to study dispersion renormalization and derive equations describing nonequilibrium dynamics of polarons by projecting equations of motion into mean-field-type wave functions. As a concrete example, we apply our method to study dynamics of impurity atoms in response to a suddenly applied force and explore the interplay of coherent Bloch oscillations and incoherent drift. We obtain a nonlinear dependence of the drift velocity on the applied force, including a sub-Ohmic dependence for small forces for dimensionality d >1 of the BEC. For the case of heavy impurity atoms, we derive a closed analytical expression for the drift velocity. Our results show considerable differences with the commonly used phenomenological Esaki-Tsu model.

  13. 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.

  14. Polaronic trapping in magnetic semiconductors

    NASA Astrophysics Data System (ADS)

    Raebiger, Hannes

    2012-02-01

    GaN doped with iron is an interesting candidate material for magnetic semiconductors, as p-d coupling between the localized Fe-d and extended N-p hole states is expected to facilitate long-range ferromagnetic alignment of the Fe spins [1]. This picture of extended states in GaN:Fe, however, falls apart due to a polaronic localization of the hole carriers nearby the Fe impurities. To elucidate the carrier localization in GaN:Fe and related iron doped III-V semiconductors, I present a systematic study using self-interaction corrected density-functional calculations [2]. These calculations predict three distinct scenarios. (i) Some systems do sustain extended host-like hole states, (ii) some exhibit polaronic trapping, (iii) and some exhibit carrier trapping at Fe-d orbitals. These behaviors are described in detail to give an insight as to how to distinguish them experimentally. I thank T. Fujita, C. Echeverria-Arrondo, and A. Ayuela for their collaboration.[4pt] [1] T. Dietl et al, Science, 287, 1019 (2000).[0pt] [2] S. Lany and A. Zunger, Phys. Rev. B, 80, 085202 (2009).

  15. 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.

  16. 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

  17. Dangling Bond Magnetic Polaron in CdSe nanocrystals

    NASA Astrophysics Data System (ADS)

    Efros, Alexander; Rodina, Anna

    In this work we study theoretically the effect of the spins of the surface dangling bonds on the PL of CdSe nanocrystals (NCs). We show that spins of dangling bonds open new recombination channels for the dark exciton recombination which is connected with flip-flip and flip-flop spin-assisted recombination of the dark exciton. Calculations show that at low temperatures the interaction between dangling bonds and NC excitons leads to the dynamical polarization of the dangling bond spins along the anisotropic axis following by the formation of a dangling bond magnetic polaron. An increase of the temperature, or of the external magnetic field perpendicular to the anisotropic axis, destroys the polaron state. This results in a shift of the transition energy and an increase of its recombination rate. Thus thermal depolarization of the polaron state may explain the small activation energies observed in the temperature dependences of the exciton lifetimes in CdSe NCs. The exchange interaction of the electron spin with spins of the surface dangling bonds explains also radiative recombination of the dark excitons in nanowires, nanorods and nanoplatelets.

  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. Importance of Polaronic Effects for Charge Transport in CdSe Quantum Dot Solids.

    PubMed

    Prodanović, Nikola; Vukmirović, Nenad; Ikonić, Zoran; Harrison, Paul; Indjin, Dragan

    2014-04-17

    We developed an accurate model accounting for electron-phonon interaction in colloidal quantum dot supercrystals that allowed us to identify the nature of charge carriers and the electrical transport regime. We find that in experimentally analyzed CdSe nanocrystal solids, the electron-phonon interaction is sufficiently strong that small polarons localized to single dots are formed. Charge-carrier transport occurs by small polaron hopping between the dots, with mobility that decreases with increasing temperature. While such a temperature dependence of mobility is usually considered as a proof of band transport, we show that the same type of dependence occurs in the system where transport is dominated by small polaron hopping. PMID:26269977

  20. 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.

  1. Circuit-QED-based superconducting quantum simulator for the Holstein-polaron model

    NASA Astrophysics Data System (ADS)

    Mei, Feng; Stojanović, Vladimir; Siddiqi, Irfan; Tian, Lin

    2014-03-01

    We propose an analog quantum simulator for the Holstein molecular-crystal model based on a superconducting circuit-QED system in the dispersive regime. The many-body Hamiltonian of this model includes both bosonic and fermionic degrees of freedom. By varying the driving field on the superconducting resonators, one can readily access both the adiabatic and anti-adiabatic regimes of this model, and reach the strong e-ph coupling limit required for small-polaron formation. We show that small-polaron state of arbitrary quasimomentum can be generated by applying a microwave pulse to the resonators. We also show that significant squeezing in the resonator modes can be achieved in the polaron-crossover regime through a measurement-based scheme. The project was supported by NSF-0956064, NSF-0916303, SNSF, NCCR QSIT, and NSF-0939514.

  2. 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.

  3. 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.

  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. 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. PMID:26451565

  6. Mobility of Holstein Polaron at Finite Temperature: An Unbiased Approach

    NASA Astrophysics Data System (ADS)

    Mishchenko, A. S.; Nagaosa, N.; De Filippis, G.; de Candia, A.; Cataudella, V.

    2015-04-01

    We present the first unbiased results for the mobility μ of a one-dimensional Holstein polaron obtained by numerical analytic continuation combined with diagrammatic and worldline Monte Carlo methods in the thermodynamic limit. We have identified for the first time several distinct regimes in the λ -T plane including a band conduction region, incoherent metallic region, an activated hopping region, and a high-temperature saturation region. We observe that although mobilities and mean free paths at different values of λ differ by many orders of magnitude at small temperatures, their values at T larger than the bandwidth become very close to each other.

  7. Polaronic pinning of vortex in magnetic superconductors and magnetic-superconducting multilayers

    NASA Astrophysics Data System (ADS)

    Lin, Shi-Zeng; Bulaevskii, Lev

    2013-03-01

    We present a new type of vortex pinning by enhancing the viscosity of vortex in magnetic superconductors with long relaxation time of magnetization and large magnetic susceptibility. In the absence of current, vortices are dressed by nonuniform magnetic polarization and form vortex-polarons. Under a small current and consequently low Lorentz force, the magnetic polarization follows the vortex motion. However, at long magnetic relaxation time of magnetization, there is additional dragging force by the magnetization besides the Bardeen-Stephen one, thus the effective viscosity of vortex is significantly enhanced resulting in suppression of dissipation. For a large current, the magnetic polarization cannot follow the vortex motion and the vortex-polaron dissociates, i.e. the magnetization and vortex become decoupled. In the IV characteristic, the decoupling transition shows as a voltage jump and can be identified as a depinning transition. The polaronic pinning mechanism successfully explains the observed enhancement of critical current in the ErNiBC superconductor at low temperatures. The polaronic pinning can be optimized in magnetic-superconducting multilayers. We show also that vortex-polaron creep is suppressed at low temperatures. This publication was made possible by funding from the Los Alamos Laboratory Directed Research and Development Program, project number 20110138ER.

  8. Optical studies of magnons, excitons and polarons in CuO{sub 2}-layer compounds

    SciTech Connect

    Kastner, M.A.; Birgeneau, R.J.

    1996-12-31

    The optical properties of undoped and lightly doped lamellar copper oxides are reviewed. In the undoped materials the absorption below the charge-transfer gap is dominated by magnetic and crystal field excitations of the CuO{sub 2} layers. The temperature dependence of the charge-transfer absorption provides evidence that free charged excitations form large polarons. However, the optical ionization energy of holes bound to acceptors is much larger than the thermal ionization energy, indicating that the bound polarons are small. The parameters extracted from optical measurements predict the Hall mobility of holes in lightly doped La{sub 2}CuO{sub 4}, with no adjustable parameters, confirming that the carriers are polarons.

  9. 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.

  10. Bose polarons in the strongly interacting regime

    NASA Astrophysics Data System (ADS)

    Hu, Ming-Guang; van de Graaff, Michael; Kedar, Dhruv; Cornell, Eric; Jin, Deborah

    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 40K impurities interacting with a BEC of 87Rb 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. This work is supported by NSF, NASA and NIST.

  11. Chiral plaquette polaron theory of cuprate superconductivity

    NASA Astrophysics Data System (ADS)

    Tahir-Kheli, Jamil; Goddard, William A., III

    2007-07-01

    Ab initio density functional calculations on explicitly doped La2-xSrxCuO4 find that doping creates localized holes in out-of-plane orbitals. A model for cuprate superconductivity is developed based on the assumption that doping leads to the formation of holes on a four-site Cu plaquette composed of the out-of-plane A1 orbitals apical Opz , planar Cud3z2-r2 , and planar Opσ . This is in contrast to the assumption of hole doping into planar Cudx2-y2 and Opσ orbitals as in the t-J model. Allowing these holes to interact with the d9 spin background leads to chiral polarons with either a clockwise or anticlockwise charge current. When the polaron plaquettes percolate through the crystal at x≈0.05 for La2-xSrxCuO4 , a Cudx2-y2 and planar Opσ band is formed. The computed percolation doping of x≈0.05 equals the observed transition to the “metallic” and superconducting phase for La2-xSrxCuO4 . Spin exchange Coulomb repulsion with chiral polarons leads to d -wave superconducting pairing. The equivalent of the Debye energy in phonon superconductivity is the maximum energy separation between a chiral polaron and its time-reversed partner. This energy separation is on the order of the antiferromagnetic spin coupling energy, Jdd˜0.1eV , suggesting a higher critical temperature. An additive skew-scattering contribution to the Hall effect is induced by chiral polarons and leads to a temperature dependent Hall effect that fits the measured values for La2-xSrxCuO4 . The integrated imaginary susceptibility, observed by neutron spin scattering, satisfies ω/T scaling due to chirality and spin-flip scattering of polarons along with a uniform distribution of polaron energy splittings. The derived functional form is compatible with experiments. The static spin structure factor for chiral spin coupling of the polarons to the undoped antiferromagnetic Cud9 spins is computed for classical spins on large two-dimensional lattices and is found to be incommensurate with a

  12. 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.

  13. Spin-polaron theory of high-{Tc} superconductivity: I, spin polarons and high-{Tc} pairing

    SciTech Connect

    Wood, R.F.

    1993-06-01

    The concept of a spin polaron is introduced and contrasted with the more familiar ionic polaron picture. A brief review of aspects of ionic bipolaronic superconductivity is given with particular emphasis on the real-space pairing and true Bose condensation characteristics. The formation energy of spin polarons is then calculated in analogy with ionic polarons. The spin-flip energy of a Cu spin in an antiferromagnetically aligned CuO{sub 2} plane is discussed. It is shown that the introduction of holes into the CuO{sub 2} planes will always lead to the destruction of long-range AF ordering due to the formation of spin polarons. The pairing of two spin polarons can be expected because of the reestablishment of local (short-range) AF ordering; the magnitude of the pairing energy is estimated using a simplified model. The paper closes with a brief discussion of the formal theory of spin polarons.

  14. Edwards polaron formation : From one to three dimensions

    NASA Astrophysics Data System (ADS)

    Chakraborty, M.; Mohanta, N.; Taraphder, A.; Min, B. I.; Fehske, H.

    2016-04-01

    Employing a self-consistent (optimized) variational diagonalization scheme, we investigate the formation of polaronic quasiparticles in a spinless fermion-boson transport model that couples the movement of charge carriers to fluctuations and correlations of a background medium. The background is parameterized by bosonic degrees of freedom. The variational fermion-boson Hilbert space is constructed to achieve high accuracy in one to three spatial dimensions with modest computational requirements. To characterize the ground-state properties of the Edwards model in the single-particle sector, we present exact numerical results for the polaron band dispersion, quasiparticle weight, Drude weight, mass enhancement, and the particle-boson correlations in a wide parameter regime. In the Edwards model, transport will be quasifree, diffusive or boson-assisted in the weakly fermion-boson coupled, fluctuation-dominated or strongly correlated regimes, respectively. Thereby correlated transport is not only assisted but also limited by the bosonic excitations. As a result, the Drude weight remains finite even in the limit of very small boson frequencies. For a strongly correlated background, closed loops are important, in any dimension, to generate a finite effective particle mass even when the free fermion has an infinite mass.

  15. Band or Polaron: The Hole Conduction Mechanism in the p-Type Spinel Rh 2ZnO4

    SciTech Connect

    Nagaraja, A. R.; Perry, N. H.; Mason, T. O.; Tang, Y.; Grayson, M.; Paudel, T. R.; Lany, S.; Zunger, A.

    2012-01-01

    Given the emerging role of oxide spinels as hole conductors, we discuss in this article the traditional vs. new methodologies of determining the type of conduction mechanism at play - localized polaronic vs. band-like transport. Applying (i) traditional small polaron analysis to our in-situ high temperature four-point conductivity and thermopower measurements, we previously found an activated mobility, which is indicative of the small polaron mechanism. However, (ii) employing the recent developments in correcting density functional methodologies for hole localization, we predict that the self-trapped hole is unstable and that Rh{sub 2}ZnO{sub 4} is instead a band conductor with a large effective mass. The hole mobility measured by high-field room temperature Hall effect also suggests band rather than polaron conduction. The apparent contradiction between the conclusion of the traditional procedure (i) and first-principles theory (ii) is resolved by taking into account in the previous transport analysis the temperature dependence of the effective density of states, which leads to the result that the mobility is actually temperature-independent in Rh{sub 2}ZnO{sub 4}. Our case study on Rh{sub 2}ZnO{sub 4} illustrates the range of experimental and theoretical approaches at hand to determine whether the transport mechanism of a semiconductor is band or small polaron conduction.

  16. Band or polaron: The hole conduction mechanism in the p-type spinel Rh2ZnO4

    SciTech Connect

    Nagaraja, Arpun R.; Perry, Nicola H.; Mason, Thomas O.; Tang, Yang; Grayson, Matthew; Paudel, Tula; Lany, Stephan; Zunger, Alex

    2011-08-05

    Given the emerging role of oxide spinels as hole conductors, we discuss in this article the traditional vs. new methodologies of determining the type of conduction mechanism at play––localized polaronic vs. band-like transport. Applying (i) traditional small polaron analysis to our in-situ high temperature four-point conductivity and thermopower measurements, we previously found an activated mobility, which is indicative of the small polaron mechanism. However, (ii) employing the recent developments in correcting density functional methodologies for hole localization, we predict that the self-trapped hole is unstable and that Rh₂ZnO₄ is instead a band conductor with a large effective mass. The hole mobility measured by high-field room temperature Hall effect also suggests band rather than polaron conduction. The apparent contradiction between the conclusion of the traditional procedure (i) and first-principles theory (ii) is resolved by taking into account in the previous transport analysis the temperature dependence of the effective density of states, which leads to the result that the mobility is actually temperature-independent in Rh₂ZnO₄. Our case study on Rh₂ZnO₄ illustrates the range of experimental and theoretical approaches at hand to determine whether the transport mechanism of a semiconductor is band or small polaron conduction.

  17. Bose polarons: Dynamical decay and RF signatures

    NASA Astrophysics Data System (ADS)

    Corson, John; Bohn, John

    2016-05-01

    Interactions of a single impurity with a quantum many-body environment are known to alter the character of the impurity, thereby forming a ``quasiparticle''. The condensed matter tradition often identifies quasiparticles as poles of a Green function in the complex plane, a notion whose sophistication sometimes obscures the underlying physics. The problem of a single quantum impurity in a Bose condensate, or Bose polaron, is an illustrative example where the meaning of the impurity Green function, and hence the quasiparticle itself, becomes especially transparent. Using direct diagonalization in a truncated Hilbert space, we examine the dynamical evolution and quasiparticle decay of the repulsive Bose polaron. This approach also allows us to simulate RF spectroscopy across a Feshbach resonance and outside the linear regime, as well as account for motional and thermal effects in a harmonic trap.

  18. 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.

  19. Magnetic polarons in MnTe layers

    NASA Astrophysics Data System (ADS)

    Schinagl, F.; Bonanni, A.; Holl, S.; Prechtl, G.; Krenn, H.

    1999-06-01

    We investigate the crossover from antiferromagnetic to ferromagnetic behaviour in semimagnetic semiconductor structures. Systems with two dimensional magnetic layers of (1 0 0)-MnTe equispatially inserted four times in a CdTe quantum well, embedded between Cd 0.75Mg 0.25Te barriers are studied in the ideal paramagnetic limit. The interaction between localized magnetic spins and quantum confined electronic states is shown to give rise to the formation of free magnetic polarons.

  20. Biopolymer hairpin loops sustained by polarons

    NASA Astrophysics Data System (ADS)

    Chakrabarti, B.; Piette, B. M. A. G.; Zakrzewski, W. J.

    2012-08-01

    We show that polarons can sustain looplike configurations in flexible biopolymers and that the size of the loops depend on both the flexural rigidity of the polymer and the electron-phonon coupling constant. In particular we show that for single stranded DNA (ssDNA) and polyacetylene such loops can have as few as seven monomers. We also show that these configurations are very stable under thermal fluctuations and so could facilitate the formation of hairpin loops of ssDNA.

  1. 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}.

  2. 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

  3. 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. PMID:22933249

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

    NASA Astrophysics Data System (ADS)

    Crooker, S. A.; Liu, F.; Kelley, M. R.; Martinez, N. J. D.; Nie, W.; Mohite, A.; Nayyar, I. H.; Tretiak, S.; Smith, D. L.; Ruden, P. P.

    2014-10-01

    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.

  5. 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.

  6. 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.

  7. All-coupling theory for the Fröhlich polaron

    NASA Astrophysics Data System (ADS)

    Grusdt, F.

    2016-04-01

    The Fröhlich model describes the interaction of a mobile impurity with a surrounding bath of phonons which leads to the formation of a quasiparticle, the polaron. In this paper an efficient renormalization group approach is presented which provides a description of Fröhlich polarons in all regimes ranging from weak to strong coupling. The extended renormalization group approach introduced here is capable of predicting ground state properties for arbitrarily small impurity masses. This allows us to obtain the full phase diagram of the Fröhlich Hamiltonian, which we present concretely for the Bogoliubov-Fröhlich model originally introduced to describe ultracold impurities in a Bose-Einstein condensate. For this model, whose regime of validity in ultracold quantum gases is the subject of debate, we benchmark our method by comparison of the ground state energy to recent diagrammatic quantum Monte Carlo calculations.

  8. 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.

  9. 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

  10. 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.

  11. 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.

  12. 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.

  13. 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.

  14. 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

  15. 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.

  16. 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

  17. Low hole polaron migration barrier in lithium peroxide

    NASA Astrophysics Data System (ADS)

    Ong, Shyue Ping; Mo, Yifei; Ceder, Gerbrand

    2012-02-01

    We present computational evidence of polaronic hole trapping and migration in lithium peroxide (Li2O2), a material of interest in lithium-air batteries. We find that the hole forms in the π* antibonding molecular orbitals of the peroxide (O22-) anion, and that this trapped hole induces significant local lattice distortion, forming a polaron. Our study finds migration barriers for the free polaron to be between 68 and 152 meV, depending on the hopping direction. This low barrier suggests that this material might not be as insulating as previously assumed, provided that the formation of carriers can be achieved. One transport limitation may arise from lithium vacancies, which we find to strongly bind to the polaron. This result, in combination with previous experimental results, suggests that electronic conductivity in this material is likely to be determined by vacancy diffusion.

  18. Amplitude and phase gratings based on spatially modulated densities of optically generated polarons in thermally reduced LiNbO3

    NASA Astrophysics Data System (ADS)

    Bruening, Hauke; Imlau, Mirco

    2011-03-01

    In thermally reduced, nominally pure LiNb O3 a variety of small polarons can be observed, being responsible for the distinct photochromic properties of this material. In this contribution we use a spatially modulated excitation of polarons for the recording of holographic gratings. These gratings inherit some of the pronounced features of the polarons like a stretched-exponential relaxation behavior with a lifetime in the ms-range. Beside amplitude gratings we also find phase gratings leading to a high diffraction efficiency in some recording and readout geometries. The origin of these phase gratings can't be explained by the classic photorefractive effect due to Fe Li or other photorefractive dopants. In contrast, our findings are discussed in the frame of a model taking into account a local change of the refractive index by the polaronic distortion of the crystal lattice. Measurements of activation energies also indicate that these gratings can be attributed to the small bound (NbLi4 +)-polaron. Financial support by Deutsche Forschungsgemeinschaft (IM 37/5-1) is gratefully acknowledged.

  19. 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

  20. 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.

  1. Numerical simulation of photoexcited polaron states in water

    NASA Astrophysics Data System (ADS)

    Zemlyanaya, E. V.; Volokhova, A. V.; Lakhno, V. D.; Amirkhanov, I. V.; Puzynin, I. V.; Puzynina, T. P.; Rikhvitskiy, V. S.; Atanasova, P. Kh.

    2015-10-01

    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.

  2. Optically induced magnetic polarons in EuTe

    SciTech Connect

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

    2013-12-04

    Direct measurements of the photoinduced magnetization in EuTe, using a two color pump-and-probe technique, are presented. The photoinduced effect was pumped using photons of above-the-bandgap energy, and detected by the Faraday rotation of a probe beam of energy below-the-bandgap. The photoinduced Faraday rotation changes sign, as expected from our model for the optically induced magnetic polaron. The EuTe spin-flop transition at low fields is also detected as a sharp step in the photoinduced Faraday rotation, and its observation provides additional supports for the photoinduced polaron model.

  3. 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.

  4. Thermal enhancement and stochastic resonance of polaron ratchets.

    PubMed

    Brizhik, L S; Eremko, A A; Piette, B M A G; Zakrzewski, W J

    2014-06-01

    We study the ratchet drift of large polarons (solitons) in molecular diatomic chains induced by unbiased time periodic electric fields at nonzero temperature below its critical value. We show that, at a nonzero temperature, the critical value of the intensity of the electric field above which the ratchet phenomenon takes place is lower than at zero temperature for the same frequency of the field. We show that there is a range of temperatures for which the polaron drift is larger than that at zero temperature. We also show that temperature decreases the value of the lowest critical period of the field. And, finally, we demonstrate that there is a stochastic resonance in a polaron ratchet, namely that there is an optimal temperature at which the polaron drift is a maximum. The values of the stochastic resonance temperature, the lowest critical values of the field intensity, and its period depend on various parameters of the system and, in particular, on the anisotropy of the chain parameters. This temperature induced decrease of the critical value of the field intensity and its period, as well as the stochastic resonance itself, may be important for practical applications of the ratchet phenomenon in systems involving conducting polymers and other low-dimensional materials. They may also be important in some biological macromolecules where the ratchet phenomenon could take place in biomotors and energy and/or charge transport. PMID:25019849

  5. Thermal enhancement and stochastic resonance of polaron ratchets

    NASA Astrophysics Data System (ADS)

    Brizhik, L. S.; Eremko, A. A.; Piette, B. M. A. G.; Zakrzewski, W. J.

    2014-06-01

    We study the ratchet drift of large polarons (solitons) in molecular diatomic chains induced by unbiased time periodic electric fields at nonzero temperature below its critical value. We show that, at a nonzero temperature, the critical value of the intensity of the electric field above which the ratchet phenomenon takes place is lower than at zero temperature for the same frequency of the field. We show that there is a range of temperatures for which the polaron drift is larger than that at zero temperature. We also show that temperature decreases the value of the lowest critical period of the field. And, finally, we demonstrate that there is a stochastic resonance in a polaron ratchet, namely that there is an optimal temperature at which the polaron drift is a maximum. The values of the stochastic resonance temperature, the lowest critical values of the field intensity, and its period depend on various parameters of the system and, in particular, on the anisotropy of the chain parameters. This temperature induced decrease of the critical value of the field intensity and its period, as well as the stochastic resonance itself, may be important for practical applications of the ratchet phenomenon in systems involving conducting polymers and other low-dimensional materials. They may also be important in some biological macromolecules where the ratchet phenomenon could take place in biomotors and energy and/or charge transport.

  6. 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.

  7. 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)

  8. 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.

  9. 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

  10. The structure of nanoscale polaron correlations in the layered manganites

    NASA Astrophysics Data System (ADS)

    Campbell, Branton

    2002-03-01

    Recent x-ray and neutron scattering experiments have uncovered nanoscale polaron correlations that play an essential role in the colossal magnetoresistive (CMR) behavior of the perovskite manganites. Short-range polaronic order decreases the charge-carrier mobility of the high-temperature paramagnetic state, and subsequently becomes unstable at the ferromagnetic transition, contributing to a pronounced resistivity decrease at T_C. In the bilayered perovskite system La_2-2xSr_1+2xMn_2O7 (0.3 < x < 0.5), weak x-ray diffuse scattering maxima reveal a one-dimensional incommensurate structural modulation with wavevector q = (0.3, 0, ± 1) and a correlation length of 10 to 30 Angstroms. A crystallographic analysis of the diffuse satellite intensities yields a longitudinal Jahn-Teller stretch mode suggestive of charge-density-wave fluctuations. Within the correlated regions, polaronic eg electrons form a striped pattern of occupied d(3x^2-r^2) orbitals. Dynamic polaron correlations of the zig-zag orbital type are also observed above TC and exhibit distinctly glassy behavior. These structures provide unique insights into the nature of strongly correlated polaronic systems. Collaborators: R. Osborn, D.N. Argyriou, S. Rosenkranz, L. Vasiliu-Doloc, J.F. Mitchell, S.K. Sinha, J.W. Lynn, C.D. Ling, Z. Islam, U. Ruett, and A. Berger. This work was supported by the U.S. DOE Office of Science contract No. W-31-109-ENG-38.

  11. 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

  12. 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

  13. Polaron luminescence in iron-doped lithium niobate

    NASA Astrophysics Data System (ADS)

    Harhira, A.; Guilbert, L.; Bourson, P.; Rinnert, H.

    2008-09-01

    Photoluminescence related to the bound polaron Nb{Li/4+} is investigated as a function of temperature and incident light intensity in iron-doped lithium niobate crystals with various iron concentrations. Experiments are done under constant-wave (CW) and pulsed illumination. Its found that the decay time is always monoexponential. The radiative lifetime, the activation energy of the nonradiative lifetime and the quenching temperature are only weakly sensitive to iron concentration. On the other hand, the magnitude of the photoluminescence signal seems strongly correlated to the Fe2+ concentration, and the superlinear regime evidenced at low CW illumination definitely confirms that polaron excitation in lithium niobate is a two-step process.

  14. 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.

  15. 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.

  16. Orbital effects of strong magnetic field on a two-dimensional Holstein polaron

    NASA Astrophysics Data System (ADS)

    Pradhan, Subhasree; Chakraborty, Monodeep; Taraphder, A.

    2016-03-01

    We investigate the orbital effects of a strong external magnetic field on the ground-state properties of a two-dimensional (2D) Holstein polaron, employing variational approaches based on exact diagonalization. From the ground-state energy and the wave function, we calculate the electron-phonon correlation function, the average phonon number, and the Drude weight and investigate the evolution of a 2D Holstein polaron as a function of the magnetic flux. Although the external magnetic field affects the polaron throughout the parameter regime, we show that the magnetic field has a stronger effect on a loosely bound (spatially extended) polaron. We also find that the magnetic field can be used as a tuning parameter, particularly for a weakly coupled polaron, to reduce the spatial extent of a large polaron.

  17. Solution of the Fröhlich polaron problem at intermediate couplings

    NASA Astrophysics Data System (ADS)

    Grusdt, Fabian; Shchadilova, Yulia E.; Rubtsov, Alexey N.; Demler, Eugene

    2015-05-01

    We develop a renormalization group approach for analyzing Fröhlich polarons and apply it to a problem of impurity atoms immersed in a Bose-Einstein condensate (BEC) 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. We show analytically that the energy of the Fröhlich polaron in a BEC is logarithmically UV divergent, and present a regularization scheme. This allows us to make predictions for the polaron energy, which can be tested in future experiments. Furthermore we calculate the effective mass of polarons and find a smooth crossover from weak to strong coupling regimes. Our method can be generalized to non-equilibrium polaron problems.

  18. Radio-frequency spectroscopy of polarons in ultracold Bose gases

    NASA Astrophysics Data System (ADS)

    Shashi, Aditya; Grusdt, Fabian; Abanin, Dmitry A.; Demler, Eugene

    2014-05-01

    Recent experimental advances enabled the realization of mobile impurities immersed in a Bose-Einstein condensate (BEC) of ultracold atoms. Here, we consider impurities with two or more internal hyperfine states, and study their radio-frequency (rf) absorption spectra, which correspond to transitions between two different hyperfine states. We calculate rf spectra for the case when one of the hyperfine states involved interacts with the BEC, while the other state is noninteracting, by performing a nonperturbative resummation of the probabilities of exciting different numbers of phonon modes. In the presence of interactions, the impurity gets dressed by Bogoliubov excitations of the BEC, and forms a polaron. The rf signal contains a δ-function peak centered at the energy of the polaron measured relative to the bare impurity transition frequency with a weight equal to the amount of bare impurity character in the polaron state. The rf spectrum also has a broad incoherent part arising from the background excitations of the BEC, with a characteristic power-law tail that appears as a consequence of the universal physics of contact interactions. We discuss both the direct rf measurement, in which the impurity is initially in an interacting state, and the inverse rf measurement, in which the impurity is initially in a noninteracting state. In the latter case, in order to calculate the rf spectrum, we solve the problem of polaron formation: a mobile impurity is suddenly introduced in a BEC, and dynamically gets dressed by Bogoliubov phonons. Our solution is based on a time-dependent variational ansatz of coherent states of Bogoliubov phonons, which becomes exact when the impurity is localized. Moreover, we show that such an ansatz compares well with a semiclassical estimate of the propagation amplitude of a mobile impurity in the BEC. Our technique can be extended to cases when both initial and final impurity states are interacting with the BEC.

  19. 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.

  20. Exciton and polaron interactions in self-assembled conjugated polymer aggregates

    NASA Astrophysics Data System (ADS)

    Grey, John K.; Thomas, Alan K.; Gao, Jian

    2015-08-01

    We study exciton coupling and interconversion between neutral and charged states of different spin in pi-stacked conjugated polymer aggregates. Rigorous self-assembly approaches are used to prepare aggregate nanofibers that permit reliable control of polymer chain conformational and packing (intra- and interchain) order within these structures. Exciton coupling can be tuned between the H- and J-aggregate limits, which has important implications for determining the fates of excitons and polarons. Single molecule intensity modulation spectroscopy was performed on individual nanofibers and large quenching depths of emissive singlet excitons by triplets are found in J-aggregate type structures. We propose that high intrachain order leads to exciton delocalization that effectively lowers singlet-triplet energy splittings thus increasing triplet yields. Exciton-polaron and polaron-polaron interactions are next investigated in both H- and J-type nanofibers where polarons are injected by charge transfer doping. We find that the enhanced intrachain order of J-aggregates enables efficient intrachain polaron transport and leads to significantly larger doping efficiencies than less ordered H-aggregates. As polaron densities increase, signatures of spin-spin interactions between polarons on adjacent chains become appreciable leading to the formation of a spinless bipolaron. Overall, these studies demonstrate the potential for controlling and directing exciton and polaron interactions via tuning of subtle intra- and interchain ordering characteristics of aggregates, which could benefit various polymeric optoelectronic applications.

  1. Observation of Fermi Polarons in a Tunable Fermi Liquid of Ultracold Atoms

    SciTech Connect

    Schirotzek, Andre; Wu, C.-H.; Sommer, Ariel; Zwierlein, Martin W.

    2009-06-12

    We have observed Fermi polarons, dressed spin-down impurities in a spin-up Fermi sea of ultracold atoms. The polaron manifests itself as a narrow peak in the impurities' rf spectrum that emerges from a broad incoherent background. We determine the polaron energy and the quasiparticle residue for various interaction strengths around a Feshbach resonance. At a critical interaction, we observe the transition from polaronic to molecular binding. Here, the imbalanced Fermi liquid undergoes a phase transition into a Bose liquid, coexisting with a Fermi sea.

  2. 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.

  3. On the LO-polaron dispersion in D dimensions

    NASA Astrophysics Data System (ADS)

    Gerlach, B.; Kalina, F.; Smondyrev, M.

    2003-05-01

    We discuss the (LO)polaron dispersion for arbitrary spatial dimension D. Firstly, we review the existing literature; recent numerical work is critically analyzed. Secondly, we derive novel upper bounds for the dispersion, which incorporate the correct behaviour of the dispersion up to third order of the coupling constant . A totally analytical evaluation is performed in the case D = 1. We compare the upper bounds with previously published lower bounds. Apart from a surrounding of zero dispersion, the relative deviation is on a few-percent scale.

  4. 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.

  5. The spin-polaron theory of high-Tc superconductivity

    NASA Astrophysics Data System (ADS)

    Mott, N. F.

    1990-01-01

    An outline is given of the model for some high-temperature superconductors which assumes that the carriers are holes in the (hybridized) oxygen 2p band and form ‘spin polarons’ with the moments on the copper atoms. A comparison is made with observations of spin polarons in Gd3-xvxS4 and with the properties of La1-xSrxVO3 in relation to those of La2-xSrxCuO4. It is assumed, following several authors, that in the superconductors the polarons form bipolarons, which are bosons, and a comparison is made with some other treatments of this hypothesis. It is proposed that in many such superconductors the boson, essentially a pair of these holes, moves in an impurity band, and that normally all the polarons (fermions) form bipolarons; the fermions repel each other on the same site (positive Hubbard U) but attract when on adjacent sites; the critical temperature Tc is then that at which the Bose gas becomes non-degenerate. In such materials a non-degenerate gas of bosons would carry the current above Tc as first suggested by Alexandrov et al. (1986). The linear increase in the resistivity above Tc is explained on this hypothesis. The effective mass of the bipolaron is, we believe, large (˜20 30me). The copper 3d9 moments in the superconducting range resonate between their two orientations as a consequence of the motion of the carriers, as they do in the description by Brinkman and Rice (1970) of highly correlated metals. Spin polarons, we believe, form only when this is so, but not in the antiferromagnetic range of x. A discussion is given of the resistivity above Tc, thermopower above Tc, and of the nature of the superconducting gap as shown by tunnelling. We confine our discussion to the materials containing copper, excluding for instance cubic Ba1-xKxBiO3, and possibly any superconductor containing bismuth, where the bosons may be Bi3+.

  6. 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.

  7. Polaronic effects in monolayer black phosphorus on polar substrates

    NASA Astrophysics Data System (ADS)

    Mogulkoc, A.; Mogulkoc, Y.; Rudenko, A. N.; Katsnelson, M. I.

    2016-02-01

    We investigate the effect of charge carrier interaction with surface optical phonons on the band properties of monolayer black phosphorus induced by polar substrates. We develop an analytical method based on the Lee-Low-Pines theory to calculate the spectrum of Fröhlich type continuum Hamiltonian in the long-wavelength limit. We examine the modification of a band gap and renormalization of effective masses due to the substrate-related polaronic effect. Our results show that an energy gap in supported monolayer black phosphorus is enlarged depending on a particular substrate and the interlayer distance z . Among the substrate considered, the largest gap broadening at z =2.5 Å is observed for the Al2O3 substrate, which is found to be ˜50 meV. Carrier-phonon coupling also renormalizes the effective masses which is more pronounced along the zigzag direction. Anisotropy of the effective masses becomes stronger by the influence of the polaronic effect corresponding to direction-dependent carrier-phonon coupling. We conclude that substrate phonons have a non-negligible effect on the static band properties of monolayer black phosphorus, which may be further exploited in its experimental and theoretical studies.

  8. 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.

  9. BLF-SSH polarons coupled to acoustic phonons in the adiabatic limit

    NASA Astrophysics Data System (ADS)

    Chandler, Carl J.; Marsiglio, F.

    2014-12-01

    We survey polaron formation in the Barisić-Labbé-Friedel and Su-Schrieffer-Heeger (BLF-SSH) model using acoustic phonons in the adiabatic limit. Multiple different numerical optimization routines and strong-coupling analytical calculations are used to find a robust ground-state energy for a wide range of coupling strengths. The electronic configuration and accompanying ionic distortions of the polaron were determined, as well as a nonzero critical coupling strength for polaron formation in two and three dimensions.

  10. Spin polarization of polaron in quasi-one dimensional organic system

    NASA Astrophysics Data System (ADS)

    Jiang, Hong; Zhang, Chao; Hu, Xuening; Hu, Guichao; Xie, Shijie

    2015-01-01

    The spin polarization of polarons in quasi-1D organic materials has been investigated by using the extended Su-Schrieffer-Heeger (SSH) model with spin-orbit coupling. Results show that the polaron is partly spin polarized, and that the electron-electron interaction and spin-orbit coupling compete with each other during the formation of spin polarization. The dependence of spin polarization on electron-phonon coupling is also revealed. Our results demonstrate that spin polarization is well correlated with polaron localization, thus providing useful guidance for exploring magnetic effects in organic materials.

  11. Polaronic mass renormalization of impurities in Bose-Einstein condensates: Correlated Gaussian-wave-function approach

    NASA Astrophysics Data System (ADS)

    Shchadilova, Yulia E.; Grusdt, Fabian; Rubtsov, Alexey N.; Demler, Eugene

    2016-04-01

    We propose a class of variational Gaussian wave functions to describe Fröhlich polarons at finite momenta. Our wave functions give polaron energies that are in excellent agreement with the existing Monte Carlo results for a broad range of interactions. We calculate the effective mass of polarons and find smooth crossover between weak- and intermediate-coupling strength. Effective masses that we obtain are considerably larger than those predicted by the mean-field method. A prediction based on our variational wave functions is a special pattern of correlations between host atoms that can be measured in time-of-flight experiments.

  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. Polaron formation in the vicinity of a narrow Feshbach resonance

    NASA Astrophysics Data System (ADS)

    Casteels, W.; Wouters, M.

    2014-10-01

    The polaronic system consisting of an impurity in a dilute Bose-Einstein condensate is considered in the presence of a narrow Feshbach resonance. For this purpose a coupled-channel model is used, which at the mean-field level predicts the formation of quasiparticles that are a superposition of the impurity and the molecular states. The impurity-boson interactions and the coupling between the open and closed channels are then considered weak and a perturbative calculation of the corrections to the mean-field results is presented. This allows us to examine the properties of the quasiparticles, such as the lifetime and the effective mass. The relation between the model parameters and the experimental parameters is determined by identifying the low-energy T matrix and applying a proper renormalization scheme.

  14. Radio frequency spectroscopy of polarons in ultracold Bose gases

    NASA Astrophysics Data System (ADS)

    Shashi, Aditya; Grusdt, Fabian; Abanin, Dmitry; Demler, Eugene

    2014-05-01

    Recent experimental advances enabled the realization of mobile impurities immersed in a Bose-Einstein condensate (BEC) of ultracold atoms. We consider impurities with two or more internal hyperfine states, and study their radio-frequency (RF) absorption spectra, which correspond to transitions between two different hyperfine states. We calculate RF spectra for the case when one of the hyperfine states involved interacts with the BEC, while the other state is non-interacting, by performing a non-perturbative resummation of the probabilities of exciting different numbers of phonon modes. We discuss both the direct RF measurement, in which the impurity is initially in an interacting state, and the inverse RF measurement, in which the impurity is initially in a non-interacting state. In the latter case, in order to calculate the RF spectrum, we solve the problem of polaron formation: a mobile impurity dynamically gets dressed by Bogoliubov phonons, using a time-dependent variational ansatz of coherent states.

  15. 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.

  16. Polaron-electron assisted giant dielectric dispersion in SrZrO3 high-k dielectric

    NASA Astrophysics Data System (ADS)

    Borkar, Hitesh; Barvat, Arun; Pal, Prabir; Shukla, A. K.; Pulikkotil, J. J.; Kumar, Ashok

    2016-06-01

    The SrZrO3 is a well known high-k dielectric constant (˜22) and high optical bandgap (˜5.8 eV) material and one of the potential candidates for future generation nanoelectronic logic elements (8 nm node technology) beyond silicon. Its dielectric behavior is fairly robust and frequency independent till 470 K; however, it suffers a strong small-polaron based electronic phase transition (Te) linking 650 to 750 K. The impedance spectroscopy measurements revealed the presence of conducting grains and grain boundaries at elevated temperature which provide energetic mobile charge carriers with activation energy in the range of 0.7 to 1.2 eV supporting the oxygen ions and proton conduction. X-ray photoemission spectroscopy measurements suggest the presence of weak non-stoichiometric O2- anions and hydroxyl species bound to different sites at the surface and bulk. These thermally activated charge carriers at elevated temperature significantly contribute to the polaronic based dielectric anomaly and conductivity. Our dielectric anomaly supports pseudo phase transition due to high degree of change in ZrO6 octahedral angle in the temperature range of 650-750 K, where electron density and phonon vibration affect the dielectric and conductivity properties.

  17. Spin relaxation via exchange with donor impurity-bound electrons

    NASA Astrophysics Data System (ADS)

    Appelbaum, Ian

    In the Bir-Aronov-Pikus depolarization process affecting conduction electrons in p-type cubic semiconductors, spin relaxation is driven by exchange with short-lived valence band hole states. We have identified an analogous spin relaxation mechanism in nominally undoped silicon at low temperatures, when many electrons are bound to dilute dopant ion potentials. Inelastic scattering with externally injected conduction electrons accelerated by electric fields can excite transitions into highly spin-orbit-mixed bound excited states, driving strong spin relaxation of the conduction electrons via exchange interaction. We reveal the consequences of this spin depolarization mechanism both below and above the impact ionization threshold, where conventional charge and spin transport are restored. Based upon: Lan Qing, Jing Li, Ian Appelbaum, and Hanan Dery, Phys Rev. B 91, 241405(R) (2015). We acknowledge support from NSF, DTRA, and ONR.

  18. Spin relaxation via exchange with donor impurity-bound electrons

    NASA Astrophysics Data System (ADS)

    Qing, Lan; Li, Jing; Appelbaum, Ian; Dery, Hanan

    2015-06-01

    At low temperatures, electrons in semiconductors are bound to shallow donor impurity ions, neutralizing their charge in equilibrium. Inelastic scattering of other externally injected conduction electrons accelerated by electric fields can excite transitions within the manifold of these localized states. Promotion of the bound electron into highly spin-orbit-mixed excited states drives a strong spin relaxation of the conduction electrons via exchange interactions, reminiscent of the Bir-Aronov-Pikus process where exchange occurs with valence band hole states. Through low-temperature experiments with silicon spin transport devices and complementary theory, we reveal the consequences of this spin depolarization mechanism both below and above the impact ionization threshold.

  19. EPR study of polarons in a conducting polymer with nondegenerate ground states: Alkali metal complexes of poly (p-phenylene) and phenylene oligomers

    SciTech Connect

    Kispert, L.D.; Joseph, J.; Miller, G.G.; Baughman, R.H.

    1984-08-15

    EPR measurements are used to characterize electronic states relevant for carrier transport in alkali metal doped poly(p-phenylene), PPP, fully deuterated poly(p-phenylene), DPPP, and phenylene oligomers. Observed spin concentrations per carbon are at least one decade higher than the Curie spin concentration for Na-doped polyacetylene. The number of these spins, which likely corresponds to polarons (mobile radical anions), is much less than the amount of alkali metal dopant, suggesting that much of the charge on the polymer chains is in bipolarons (spinless dianions). Relevant to the interaction between spins on the polymer chain and the metal cations, the observed g values are close to the free electron value and do not substantially vary with the donor dopant, temperature, or the molecular weight of the phenylene chain. Although the spin-orbit effect on g values is small, room temperature linewidth tends to increase with increasing atomic number of dopant: suggesting some interaction, albeit a smaller magnitude effect than for alkali-metal graphite complexes. The EPR linewidths are exchange narrowed and proton hyperfine broadening is significant. The latter explains the generally broader linewidths for doped PPP than for doped DPPP. The measured susceptibilities have a temperature dependence which suggests equilibrium between separated polaron defects and singlet and triplet spin states formed intermolecularly via polaron pairing. The interaction is antiferromagnetic and the binding energy between polarons is about 2.2 to 3.3 meV. An upper limit estimate of the Fermi-surface density of states for K-doped PPP (0.7 states/eV phenyl) is derived from an upper limit estimate of Pauli susceptibility.

  20. 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.

  1. Variational polaron self-interaction-corrected total-energy functional for charge excitations in insulators

    NASA Astrophysics Data System (ADS)

    Sadigh, Babak; Erhart, Paul; Ã berg, Daniel

    2015-08-01

    We conduct a detailed investigation of the polaron self-interaction (pSI) error in standard approximations to the exchange-correlation (XC) functional within density-functional theory (DFT). The pSI leads to delocalization error in the polaron wave function and energy, as calculated from the Kohn-Sham (KS) potential in the native charge state of the polaron. This constitutes the origin of the systematic failure of DFT to describe the polaron formation in band insulators. It is shown that the delocalization error in these systems is, however, largely absent in the KS potential of the closed-shell neutral charge state. This leads to a modification of the DFT total-energy functional that corrects the pSI in the XC functional. The resulting pSIC-DFT method constitutes an accurate parameter-free ab initio methodology for calculating polaron properties in insulators at a computational cost that is orders of magnitude smaller than hybrid XC functionals. Unlike approaches that rely on parametrized localized potentials such as DFT+U , the pSIC-DFT method properly captures both site and bond-centered polaron configurations. This is demonstrated by studying formation and migration of self-trapped holes in alkali halides (bond-centered) as well as self-trapped electrons in an elpasolite compound (site-centered). The pSIC-DFT approach consistently reproduces the results obtained by hybrid XC functionals parametrized by DFT+G0W0 calculations. Finally, we generalize the pSIC approach to hybrid functionals, and show that in stark contrast to conventional hybrid calculations of polaron energies, the pSIC-hybrid method is insensitive to the parametrization of the hybrid XC functional. On this basis, we further rationalize the success of the pSIC-DFT approach.

  2. Polaronic discontinuities induced by off-diagonal coupling

    NASA Astrophysics Data System (ADS)

    Zhang, Yuyu; Duan, Liwei; Chen, Qinghu; Zhao, Yang

    2012-07-01

    In this paper, we study a form of the Holstein molecular crystal model in which the influence of lattice vibrations on the transfers of electronic excitations between neighboring sites (off-diagonal coupling) is taken into account. Using the Toyozawa Ansatz and the Lanczos algorithm, the Holstein Hamiltonian with two types of off-diagonal coupling is studied focusing on a number of analyticity issues in the ground state. For finite-sized lattices and antisymmetric coupling, a sequence of discontinuities are found in the polaron energy dispersion, the size of the ground-state phonon cloud, and the linearized von Neumann entropy used to quantify the quantum entanglement between the exciton and the phonons in the ground state. Such behavior is accompanied by a shift of the ground-state crystal momentum from zero to nonzero values as the coupling strength is increased. In the thermodynamic limit, all discontinuities associated with antisymmetric coupling vanish except the one corresponding to the initial departure of the ground-state wavevector from the Brillouin zone center. For the case of symmetric off-diagonal coupling, a smooth crossover is found to exist in all parameters regimes.

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

    PubMed

    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

  4. Polaronic discontinuities induced by off-diagonal coupling.

    PubMed

    Zhang, Yuyu; Duan, Liwei; Chen, Qinghu; Zhao, Yang

    2012-07-21

    In this paper, we study a form of the Holstein molecular crystal model in which the influence of lattice vibrations on the transfers of electronic excitations between neighboring sites (off-diagonal coupling) is taken into account. Using the Toyozawa Ansatz and the Lanczos algorithm, the Holstein Hamiltonian with two types of off-diagonal coupling is studied focusing on a number of analyticity issues in the ground state. For finite-sized lattices and antisymmetric coupling, a sequence of discontinuities are found in the polaron energy dispersion, the size of the ground-state phonon cloud, and the linearized von Neumann entropy used to quantify the quantum entanglement between the exciton and the phonons in the ground state. Such behavior is accompanied by a shift of the ground-state crystal momentum from zero to nonzero values as the coupling strength is increased. In the thermodynamic limit, all discontinuities associated with antisymmetric coupling vanish except the one corresponding to the initial departure of the ground-state wavevector from the Brillouin zone center. For the case of symmetric off-diagonal coupling, a smooth crossover is found to exist in all parameters regimes. PMID:22830684

  5. Energy spectrum of the optical polaron at finite total momentum

    NASA Astrophysics Data System (ADS)

    Gerlach, B.; Kalina, F.

    1999-10-01

    In the following discussion we are concerned with the standard Fröhlich model for an optical polaron. We clarify the qualitative properties of the energy spectrum for arbitrary total momentum Q. Concerning the ground-state energy, we establish an effective lower bound. Until now, we have to assume that the electron-phonon coupling parameter α does not exceed a specified positive value. Using this bound, we demonstrate that the ground-state energy coincides with the continuum edge for \\|Q\\|>=\\|QC\\|, QC being finite. Consequently, it is only for \\|Q\\|<\\|QC\\| that an isolated ground state exists at all. This behavior is strikingly different from that of the corresponding system in lower dimensions, which has been analyzed previously by other authors, the discussion of the three-dimensional case remaining incomplete. Concerning the overall behavior of the ground-state energy as a function of Q and α, we find an increase (strict decrease) with increasing \\|Q\\|(α). In addition, we present an approach to the excited states. Interestingly enough, this can be based entirely on the knowledge of the ground-state energy and ground-state wave function.

  6. Polaronic absorption in Sr2IrO4

    NASA Astrophysics Data System (ADS)

    Sohn, Chang Hee; Qi, Tong-Fei; Noh, Kyung Joo; Park, Hyun-Ju; Yoo, Hyang Keun; Cao, Gang; Kim, Kyung Wan; Cho, Deok-Yong; Moon, Soon Jae; Noh, Tae Won

    2014-03-01

    Sr2IrO4 has received much attention as a novel Jeff = 1/2 Mott insulator. Many theorists have supposed that exotic novel ground state such as superconductivity, topological insulator, and quantum spin liquid could emerge in Jeff = 1/2 state. However, despite of great interests on Sr2IrO4, the ground state of this material is elusive up to now. Unlike previous Mott scenario, recent reports support that Sr2IrO4 can be described as Slater insulator rather than Mott insulator. The origin of temperature evolutions of electronic structure shown in many experiments also remains vague until now. Here, we investigated the detail temperature evolution of electronic structure of Sr2IrO4 using infrared spectroscopy. We couldn't observe any anomaly in optical conductivity near the TN, which is not consistent with recent reports. Instead, we observed the continuous changes in our optical data which can be explained in terms of polaronic behavior, closely related to La2CuO4.

  7. Liquid-state polaron theory of the hydrated electron revisited

    NASA Astrophysics Data System (ADS)

    Donley, James P.; Heine, David R.; Tormey, Caleb A.; Wu, David T.

    2014-07-01

    The quantum path integral/classical liquid-state theory of Chandler and co-workers, created to describe an excess electron in solvent, is re-examined for the hydrated electron. The portion that models electron-water density correlations is replaced by two equations: the range optimized random phase approximation (RO-RPA), and the Donley, Rajasekaran, and Liu (DRL) approximation to the "two-chain" equation, both shown previously to describe accurately the static structure and thermodynamics of strongly charged polyelectrolyte solutions. The static equilibrium properties of the hydrated electron are analyzed using five different electron-water pseudopotentials. The theory is then compared with data from mixed quantum/classical Monte Carlo and molecular dynamics simulations using these same pseudopotentials. It is found that the predictions of the RO-RPA and DRL-based polaron theories are similar and improve upon previous theory, with values for almost all properties analyzed in reasonable quantitative agreement with the available simulation data. Also, it is found using the Larsen, Glover, and Schwartz pseudopotential that the theories give values for the solvation free energy that are at least three times larger than that from experiment.

  8. Liquid-state polaron theory of the hydrated electron revisited

    SciTech Connect

    Donley, James P.; Heine, David R.; Tormey, Caleb A.; Wu, David T.

    2014-07-14

    The quantum path integral/classical liquid-state theory of Chandler and co-workers, created to describe an excess electron in solvent, is re-examined for the hydrated electron. The portion that models electron-water density correlations is replaced by two equations: the range optimized random phase approximation (RO-RPA), and the Donley, Rajasekaran, and Liu (DRL) approximation to the “two-chain” equation, both shown previously to describe accurately the static structure and thermodynamics of strongly charged polyelectrolyte solutions. The static equilibrium properties of the hydrated electron are analyzed using five different electron-water pseudopotentials. The theory is then compared with data from mixed quantum/classical Monte Carlo and molecular dynamics simulations using these same pseudopotentials. It is found that the predictions of the RO-RPA and DRL-based polaron theories are similar and improve upon previous theory, with values for almost all properties analyzed in reasonable quantitative agreement with the available simulation data. Also, it is found using the Larsen, Glover, and Schwartz pseudopotential that the theories give values for the solvation free energy that are at least three times larger than that from experiment.

  9. 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.

  10. Coupled polaronic and ion transport in nanocrystalline metal oxide electrodes

    NASA Astrophysics Data System (ADS)

    Rosso, Kevin

    2012-02-01

    We report new computational methods and fundamental understanding in the dynamics of coupled charge and ion transport in nanoscale metal oxides. The methods attack the multi-scale problem of simulating the collective diffusivities of ions and charge compensating e-/h+ carriers in single crystal particles, across particle-particle grain boundaries, and through networks of grains for select systems. Methods include embedded quantum mechanical clusters at the DFT and MP2 levels of theory for atomic-scale polaronic and ion transport kinetics, classical DFT-based free energy calculations for grain-scale conductivity in the framework of the Poisson-Nernst-Planck formalism, and phase field simulation of charged particle diffusivity for conductivity at the grain network scale. This combination of approaches is one of a kind in terms of its multi-scale range, scaling, and computational efficiency. We are presently focused on coupled electron and Li+ ion transport in polymorphs of TiO2, and also in mixed valence spinel oxides, for electrode conductivity optimization and improving energy storage materials performance for Li+ batteries.

  11. Polaronic Superlattice Formed on Oxidised Magnetite (111) Surface

    NASA Astrophysics Data System (ADS)

    Berdunov, N.; Mariotto, G.; Murphy, S.; Ceballos, S. F.; Jordan, K.; Shvets, I. V.

    2003-12-01

    We present direct experimental evidence of the formation of a superstructure on the (111) surface of a magnetite, Fe3O4 single crystal. The superstructure, which has a periodicity of 42 A and three-fold symmetry has been observed by means of STM and LEED. Under the correct conditions of oxygen pressure and sample anneal temperature the superstructure is reproducibly formed throughout most of the sample surface. The characteristics of the superstructure, including its dependency on the tunnel bias voltage and its atomic scale periodicity, suggest that it is an electronic effect rather than a mosaic of several iron oxide phases. We explain the results in terms of the formation of giant static polarons, although we notice that other types of electron-lattice instabilities such as charge density wave may offer possible explanations. We suggest two possible scenarios of instability linking the electron band structure and lattice distortions in magnetite: either resulting from reallocation of Fe2+ and Fe3+ valence states between octahedral sites or alternatively from reallocation between octahedral and tetrahedral sites.

  12. Light induced polaron formation in perovskite solar cell devices

    NASA Astrophysics Data System (ADS)

    Neukirch, Amanda; Nie, Wanyi; Blancon, Jean-Christophe; Appavoo, Kannatassen; Tsai, Hsinhan; Chhowalla, Manish; Alam, Muhammad; Sfeir, Matthew; Katan, Claudine; Even, Jacky; Crochet, Jared; Gupta, Gautum; Mohite, Aditya; Tretiak, Sergei

    The need for a low-cost, clean, and abundant source of energy has generated large amounts of research in solution processed solar cell materials. The lead halide perovskite has rapidly developed as a serious candidate for the active layer of photovoltaic devices. The efficiencies of devices made with this material have increased from 3.5% to over 20% in around 5 years. Despite the remarkable progress associated with perovskite materials, there are still fundamental questions regarding their lack of photo-stability over prolonged solar irradiation that need to be addressed. Recent experiments on photo-degradation under constant illumination have found fast self-healing by resting the device in the dark for less than 1 minute. Density functional theory and symmetry analysis show that localized charge states couple to local structural lattice distortions and methyl ammonium quasistatic configurations. Once translational symmetry is lost, additional bonding configurations become symmetry allowed, triggering localized charges in the vicinity over time under constant illumination, thus seeding the formation of macroscopic charged domains and preventing efficient charge extraction. Here we present an in-depth study of polaron formation and binding energy at the atomistic level.

  13. Interferometric measurement of many-body topological invariants using polarons

    NASA Astrophysics Data System (ADS)

    Grusdt, Fabian; Yao, Norman; Abanin, Dmitry; Demler, Eugene

    2014-05-01

    We present a scheme for the direct detection of many-body topological invariants in ultra cold quantum gases in optical lattices. We generalize single-particle interferometric schemes developed for the detection of topologically non-trivial band structures [Atala et al., Nature Physics 9, 795 (2013)] by coupling a spin-1/2 impurity to a (topological) excitation of an interacting many-body system. Performing Ramsey interferometry in combination with Bloch oscillations of the resulting polaronic particle allows to directly detect the many body-topological invariant. In particular we consider adiabatic Thouless pumps in the super-lattice Bose-Hubbard model, which transport a quantized amount of particles across a one-dimensional lattice. In the presence of inter-atomic interactions this quantized current is given by a many-body Chern number, which can be measured using our protocol. These systems also support symmetry-protected topological phases, the invariants of which can be obtained from our protocol as well.

  14. 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

  15. Charge localization in a layer induced by electron-phonon interaction: application to transient polaron formation

    NASA Astrophysics Data System (ADS)

    Li, Guangqi; Movaghar, Bijan

    2015-06-01

    We describe electron transfer and localization in a finite two-dimensional transporting layer (15 × 15) using a tight binding Hamiltonian where each site is coupled to phonons. For a narrow electronic band, a polaron is formed with a population that peaks in the middle of the layer and exhibits a concomitant energy lowering. A "local defect" can be simulated by lowering or raising the corresponding site energy. As an example, if we put the defect in one corner, the consequence is that the electron population builds up a polaron which is repelled from this region. The model has been applied to describe the experimentally observed real time polaron formation process in organic layers and in particular in the surface bands of ice-covered metal. We simulate the polaron formation, population distribution and energy relaxation in time. We also investigate the effect of local fluctuations on polaron formation. The formalism can be generalized to excitonic trapping, and has many potential applications. Supplementary material in the form of one pdf file available from the Journal web page at: http://dx.doi.org/10.1140/epjb/e2015-60258-3.

  16. 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

  17. 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.

  18. First-principles study of hole polaron formation and migration in SrI2

    NASA Astrophysics Data System (ADS)

    Zhou, Fei; Sadigh, Babak; Aberg, Daniel

    2015-03-01

    We investigate the formation of self-trapped holes (STH) in the high performance scintillator material SrI2 using a recently developed first principles method, polaron self-interaction correction (pSIC). pSIC removes the significant spurious self-interaction of localized polaron states. It is capable of accurately reproduce the configurational energy landscape of polaronic states from optimized hybrid functionals at the computational cost of the local density approximation. We searched for and identified all symmetrically distinct STH states localized on neighboring I-I dimers, i.e. Vk centers, and found non-trivial relation between the STH formation energies and dimer separation. All possible polaron hopping paths of the type IAIB -->IBIC are investigated systematically with pSIC and the elastic band method, and paths with low migration barrier energy of about 0.2 eV were identified, suggesting high mobility in SrI2. We expect that the present approach can be applied to study polaron formation and migration in other materials. Support from the National Nuclear Security Administration Office of Nonproliferation Research and Development (NA-22) is acknowledged. This work performed under the auspices of the U.S. Department of Energy by Lawrence Livermore N We acknowledge funding from the NA-22 agency.

  19. 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

  20. 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.

  1. Ultralong-Range Polaron-Induced Quenching of Excitons in Isolated Conjugated Polymers

    NASA Astrophysics Data System (ADS)

    Bolinger, Joshua C.; Traub, Matthew C.; Adachi, Takuji; Barbara, Paul F.

    2011-02-01

    In conjugated polymers, radiative recombination of excitons (electron-hole pairs) competes with nonradiative thermal relaxation pathways. We visualized exciton quenching induced by hole polarons in single-polymer chains in a device geometry. The distance-scale for quenching was measured by means of a new subdiffraction, single-molecule technique—bias-modulated intensity centroid spectroscopy—which allowed the extraction of a mean centroid shift of 14 nanometers for highly ordered, single-polymer nanodomains. This shift requires energy transfer over distances an order of magnitude greater than previously reported for bulk conjugated polymers and far greater than predicted by the standard mechanism for exciton quenching, the unbiased diffusion of free excitons to quenching sites. Instead, multistep “energy funneling” to trapped, localized polarons is the probable mechanism for polaron-induced exciton quenching.

  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. Improving Li2O2 conductivity via polaron preemption: An ab initio study of Si doping

    NASA Astrophysics Data System (ADS)

    Timoshevskii, Vladimir; Feng, Zimin; Bevan, Kirk H.; Goodenough, John; Zaghib, Karim

    2013-08-01

    We report on ab initio electronic structure simulations of Li2O2, where 1.6% of lithium atoms are substituted by silicon. It is demonstrated that this leads to the formation of conducting impurity states in the band gap of Li2O2. We show that these states originate from the antibonding orbitals of the oxygen pairs and are remarkably stable against possible polaron formation (upon electron injection). Through this polaron preemption mechanism, the proposed compound is expected to show significantly higher electronic mobility than stoichiometric Li2O2, which could have significant applications in lithium-air batteries.

  4. 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.

  5. 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.

  6. 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.

  7. 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.

  8. 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.

  9. 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.

  10. 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.

  11. Characterization of iron substitution process in Fe:LiNbO 3 single crystal fibers by polaron measurements

    NASA Astrophysics Data System (ADS)

    Bourson, P.; Aillerie, M.; Cochez, M.; Ferriol, M.; Zhang, Y.; Guilbert, L.

    2003-10-01

    The growth of iron-doped single-crystal fibers of lithium niobate was performed by the Laser Heated Pedestal Growth Technique for different Fe 2O 3 contents in the feed rods. We used the polaron luminescence to explain the processes of iron substitution in iron-doped single-crystal fibers of lithium niobate. The interpretation of the polaron behavior as a function of iron concentration confirms several predicted effects as the decrease of the global amount of vacancies and the predominant role of the niobium in its polaronic or bipolaronic forms in the LN lattice.

  12. Magnetic field effects in singlet-polaron quenching in molecularly doped fluorescence organic light-emitting diodes

    NASA Astrophysics Data System (ADS)

    Xu, Kai; Ma, Dongge

    2014-08-01

    The magnetic field effects of electroluminescence (MEL) in 4-[dicyanomethylene]-2-t-butyl-6-(1,1,7,7-tetramethyljulolidyl-9-enyl)-4H-pyran(DCJTB) doped tri-(8-hydroxyquinoline)-aluminum (Alq3) based organic light-emitting diodes were investigated. A linear decrease in MEL with the increase of magnetic field was observed at high magnetic field (>20 mT) in this doping devices, which has been attributed to the singlet-polaron quenching effect. It was found that the singlet-polaron quenching is magnetic field dependent. Our results showed that singlet-polaron quenching commonly exists in fluorescence OLEDs and induces the linear decrease in MEL.

  13. 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

  14. 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.

  15. Zero-Magnetic-Field Spin Splitting of Polaron's Ground State Energy Induced by Rashba Spin-Orbit Interaction

    NASA Astrophysics Data System (ADS)

    Liu, Jia; Xiao, Jing-Ling

    2006-10-01

    We study theoretically the ground state energy of a polaron near the interface of a polar-polar semiconductor by considering the Rashba spin-orbit (SO) coupling with the Lee-Low-Pines intermediate coupling method. Our numerical results show that the Rashba SO interaction originating from the inversion asymmetry in the heterostructure splits the ground state energy of the polaron. The electron areal density and vector dependence of the ratio of the SO interaction to the total ground state energy or other energy composition are obvious. One can see that even without any external magnetic field, the ground state energy can be split by the Rashba SO interaction, and this split is not a single but a complex one. Since the presents of the phonons, whose energy gives negative contribution to the polaron's, the spin-splitting states of the polaron are more stable than electron's.

  16. 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.

  17. 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

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

    PubMed

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

    2015-01-01

    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

  19. Conventional versus unconventional magnetic polarons: ZnMnTe/ZnSe and ZnTe/ZnMnSe quantum dots

    NASA Astrophysics Data System (ADS)

    Barman, B.; Tsai, Y.; Scrace, T.; Murphy, J. R.; Cartwright, A. N.; Pientka, J. M.; Zutic, I.; McCombe, B. D.; Petrou, A.; Sellers, I. R.; Oszwaldowski, R.; Petukhov, A.; Fan, W. C.; Chou, W. C.; Yang, C. S.

    2014-08-01

    We used time resolved photoluminescence (TRPL) spectroscopy to compare the properties of magnetic polarons in two related, spatially indirect, II-VI epitaxially grown quantum dot systems. In sample A (ZnMnTe/ZnSe), the photoexcited holes are confined in the magnetic ZnMnTe quantum dots (QDs), while the electrons remain in the surrounding non-magnetic ZnSe matrix. In sample B (ZnTe/ZnMnSe) on the other hand, the holes are confined in the non-magnetic ZnTe QDs and the electrons move in the magnetic ZnMnSe matrix. The magnetic polaron formation energies, EMP , in these samples were measured from the temporal red-shift of the excitonic emission peak. The magnetic polarons in the two samples exhibit distinct characteristics. In sample A, the magnetic polaron is strongly bound with EMP=35 meV. Furthermore, EMP has unconventionally weak dependence of on both temperature T and magnetic field Bappl . In contrast, magnetic polarons in sample B show conventional characteristics with EMP decreasing with increasing temperature and increasing external magnetic field. We attribute the difference in magnetic polaron properties between the two types of QDs to the difference in the location of the Mn ions in the respective structures.

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

    NASA Astrophysics Data System (ADS)

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

    2015-07-01

    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.

  1. 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.

  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. Spin Relaxation of an Impurity Polaron in a Parabolic Quantum Dot

    NASA Astrophysics Data System (ADS)

    Li, Zhi-Xin

    2015-01-01

    We have studied theoretically the spin relaxation of an impurity polaron, which arises from the electron interactions with the longitudinal optical phonon between the sublevel Zeeman splitting of the ground-state, by employing a variational method for a parabolic quantum dot (QD). In fact, this process occurs by the absorption of a deformation potential acoustic phonon. With Rashba spin-orbit coupling, the expression of the spin relaxation rate of an impurity polaron as functions of the radius of QD, the Lande factor parameter, the magnetic field adjusting length has been derived. Results of the numerical calculation show that the spin relaxation rate decreases with increasing the radius of QD and enlarges with increasing the magnetic field adjusting length when the magnetic field adjusting length . In addition, we find that the spin relaxation rate is an increasing function of the Lande factor parameter.

  4. Polaron Coherence Condensation As the Mechanism for Colossal Magnetoresistance in Layered Manganites

    SciTech Connect

    Mannella, N.; Yang, W.L.; Tanaka, K.; Zhou, X.J.; Zheng, H.; Mitchell, J.F.; Zaanen, J.; Devereaux, T.P.; Nagaosa, N.; Hussain, Z.; Shen, Z.-X.; /SLAC

    2007-11-20

    Angle-resolved photoemission spectroscopy data for the bilayer manganite La{sub 1.2}Sr{sub 1.8}Mn{sub 2}O{sub 7} show that, upon lowering the temperature below the Curie point, a coherent polaronic metallic groundstate emerges very rapidly with well defined quasiparticles which track remarkably well the electrical conductivity, consistent with macroscopic transport properties. Our data suggest that the mechanism leading to the insulator-to-metal transition in La{sub 1.2}Sr{sub 1.8}Mn{sub 2}O{sub 7} can be regarded as a polaron coherence condensation process acting in concert with the Double Exchange interaction.

  5. 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.

  6. 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.

  7. Mapping polarons in polymer FETs by charge modulation microscopy in the mid-infrared

    PubMed Central

    Chin, Xin Yu; Yin, Jun; Wang, Zilong; Caironi, Mario; Soci, Cesare

    2014-01-01

    We implemented spatial mapping of charge carrier density in the channel of a conventional polymer Field-Effect Transistor (FET) by mid-infrared Charge Modulation Spectroscopy (CMS). CMS spectra are recorded with a high sensitivity confocal Fourier Transform Infra-Red (FTIR) microscope by probing electroinduced Infra-Red Active Vibrational (IRAV) modes and low-energy polaron bands in the spectral region 680–4000 cm−1. Thanks to the high specificity and strong oscillator strength of these modes, charge-induced reflectance measurements allow quantitative estimation of charge carrier densities within the FET channel, without the need for amplitude or phase modulation. This is illustrated by identifying the contribution of intrinsic and electrostatically induced polarons to conduction, and by mapping the polaron spatial distribution in a P3HT (Poly(3-hexylthiophene-2,5-diyl)) FET channel under different drain-source bias conditions. This work demonstrates the potential of mid-infrared charge modulation microscopy to characterize carrier injection and transport in semiconducting polymer materials. PMID:24406635

  8. 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.

  9. Resistive transition, polaron dynamics and scaling behavior in Fe doped SrTiO3

    NASA Astrophysics Data System (ADS)

    Ghosh, Arijit; Masud, Md. G.; Sannigrahi, Jhuma; Chaudhuri, B. K.

    2013-04-01

    Temperature dependent electrical transport (ac and dc) and dielectric measurements have been performed with SrFexTi(1-x)O3 (0≤x≤1.0) samples prepared by ceramic route. Metal-insulator like transition observed depending on doping concentration. High dc resistivity of the present system is due to localization of polaronic charge carriers and the dc resistivity data, above respective TMI, fit well with Mott's variable range hopping, Arrhenius conduction mechanism, while a power law nature is followed below TMI. The charge transport mechanism is also revealed from the scaled ac conductivity and dielectric modulus spectrum. The MI transition is considered to be associated with polaron dissociation occurring little below polaron ordering (PO) temperature, TPO. The samples also indicate a cross-over from universal dielectric response (UDR) (f<105 Hz) to second universality (SU) (f>105 Hz). This cross over as well as MI like transition temperature shift towards the lower temperature regime with increasing x.

  10. Mapping polarons in polymer FETs by charge modulation microscopy in the mid-infrared

    NASA Astrophysics Data System (ADS)

    Chin, Xin Yu; Yin, Jun; Wang, Zilong; Caironi, Mario; Soci, Cesare

    2014-01-01

    We implemented spatial mapping of charge carrier density in the channel of a conventional polymer Field-Effect Transistor (FET) by mid-infrared Charge Modulation Spectroscopy (CMS). CMS spectra are recorded with a high sensitivity confocal Fourier Transform Infra-Red (FTIR) microscope by probing electroinduced Infra-Red Active Vibrational (IRAV) modes and low-energy polaron bands in the spectral region 680-4000 cm-1. Thanks to the high specificity and strong oscillator strength of these modes, charge-induced reflectance measurements allow quantitative estimation of charge carrier densities within the FET channel, without the need for amplitude or phase modulation. This is illustrated by identifying the contribution of intrinsic and electrostatically induced polarons to conduction, and by mapping the polaron spatial distribution in a P3HT (Poly(3-hexylthiophene-2,5-diyl)) FET channel under different drain-source bias conditions. This work demonstrates the potential of mid-infrared charge modulation microscopy to characterize carrier injection and transport in semiconducting polymer materials.

  11. Electron Spin Relaxation of Hole and Electron Polarons in π-Conjugated Porphyrin Arrays: Spintronic Implications.

    PubMed

    Rawson, Jeff; Angiolillo, Paul J; Frail, Paul R; Goodenough, Isabella; Therien, Michael J

    2015-06-18

    Electron spin resonance (ESR) spectroscopic line shape analysis and continuous-wave (CW) progressive microwave power saturation experiments are used to probe the relaxation behavior and the relaxation times of charged excitations (hole and electron polarons) in meso-to-meso ethyne-bridged (porphinato)zinc(II) oligomers (PZnn compounds), which can serve as models for the relevant states generated upon spin injection. The observed ESR line shapes for the PZnn hole polaron ([PZnn](+•)) and electron polaron ([PZnn](-•)) states evolve from Gaussian to more Lorentzian as the oligomer length increases from 1.9 to 7.5 nm, with solution-phase [PZnn](+•) and [PZnn](-•) spin-spin (T2) and spin-lattice (T1) relaxation times at 298 K ranging, respectively, from 40 to 230 ns and 0.2 to 2.3 μs. Notably, these very long relaxation times are preserved in thick films of these species. Because the magnitudes of spin-spin and spin-lattice relaxation times are vital metrics for spin dephasing in quantum computing or for spin-polarized transport in magnetoresistive structures, these results, coupled with the established wire-like transport behavior across metal-dithiol-PZnn-metal junctions, present meso-to-meso ethyne-bridged multiporphyrin systems as leading candidates for ambient-temperature organic spintronic applications. PMID:25697578

  12. Time-resolved photoluminescence spectroscopy of NbNb4 + and O- polarons in LiNbO3 single crystals

    NASA Astrophysics Data System (ADS)

    Kämpfe, T.; Haußmann, A.; Eng, L. M.; Reichenbach, P.; Thiessen, A.; Woike, T.; Steudtner, R.

    2016-05-01

    We probe here the optical relaxation properties of Mg-doped wide-band-gap LiNbO3 single crystals with both a high spectral and temporal resolution at cryogenic temperatures. Surprisingly, we observe the photoluminescence to decay in a two-step process: a fast relaxation and a slower one centered around an energy Emax = 2.62 ±0.05 eV. Both decays fit well to the stretched-exponential behavior. Moreover, we are able to associate these energies to the recombination of light-induced NbNb4 + and O- small polarons. Also, we checked the stability of our findings by using LiNbO3 single crystals that show on-purpose modified radiative recombination processes, i.e., with a Mg doping both above and below the optical damage resistance threshold, as well as with different poling histories of inverted domains.

  13. Response of the polaron system consisting of an impurity in a Bose-Einstein condensate to Bragg spectroscopy

    NASA Astrophysics Data System (ADS)

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

    2011-03-01

    We expand the existing polaron response theory, expressed within the Mori-Zwanzig projection operator formalism applicable for the transfer of arbitrary energy and zero momentum, for the case of finite momentum exchange. A general formula is then derived that can be used to calculate the response of a system to a probe that transfers both momentum and energy to the system. The main extension of the existing polaron response theory is the finite momentum exchange, which was not needed until now, since it is negligible for optical absorption. However, this formalism is needed to calculate the response of the polaronic system consisting of an impurity in a Bose-Einstein condensate (BEC) to Bragg spectroscopy. We show that the well-known features that appear in the optical absorption of the solid-state Fröhlich polaron are also present in the Bragg response of the BEC-impurity polaron. The f-sum rule is written in a form suitable to provide an independent consistency test for our results. The effect of lifetime broadening on the BEC-impurity spectrum is examined. The results derived here are discussed in the framework of an experimental realization consisting of a lithium impurity in a sodium condensate.

  14. Acceptor and Excitation Density Dependence of the Ultrafast Polaron Absorption Signal in Donor-Acceptor Organic Solar Cell Blends.

    PubMed

    Zarrabi, Nasim; Burn, Paul L; Meredith, Paul; Shaw, Paul E

    2016-07-21

    Transient absorption spectroscopy on organic semiconductor blends for solar cells typically shows efficient charge generation within ∼100 fs, accounting for the majority of the charge carriers. In this Letter, we show using transient absorption spectroscopy on blends containing a broad range of acceptor content (0.01-50% by weight) that the rise of the polaron signal is dependent on the acceptor concentration. For low acceptor content (<10% by weight), the polaron signal rises gradually over ∼1 ps with most polarons generated after 200 fs, while for higher acceptor concentrations (>10%) most polarons are generated within 200 fs. The rise time in blends with low acceptor content was also found to be sensitive to the pump fluence, decreasing with increasing excitation density. These results indicate that the sub-100 fs rise of the polaron signal is a natural consequence of both the high acceptor concentrations in many donor-acceptor blends and the high excitation densities needed for transient absorption spectroscopy, which results in a short average distance between the exciton and the donor-acceptor interface. PMID:27355877

  15. Detailed relationship between local structure, polarons, and magnetizationfor La1-xCaxMnO3 (0.21≤x≤0.45)

    NASA Astrophysics Data System (ADS)

    Bridges, F.; Downward, L.; Neumeier, J. J.; Tyson, T. A.

    2010-05-01

    We present detailed local structure measurements (using the extended x-ray absorption fine structure technique) for the colossal magnetoresistive material La1-xCaxMnO3 (0.21polaron and Jahn-Teller (JT) distortions, σJT/polaron2 , are a universal function of the magnetization, independent of how the magnetization is achieved via changes in temperature or magnetic field. However this universal behavior is only observed for Bfields≥2T , likely as a result of domain canting in low B fields. The resulting curve is well described by two straight lines with significantly different slopes. These regimes represent two distinctly differ distortions of the oxygen octahedra about the Mn. For low magnetizations up to ˜65% of the theoretical maximum magnetization, MT , the slope is low and the distortion removed as the sample becomes magnetized is small—we argue this arises from polarons which have a low distortion around two (or possibly three) Mn sites. At high magnetizations large distortions per Mn site are removed as these sites become magnetized. The data are also analyzed in terms of a two Mn-O peak distribution using experimental standards for Mn-O. The results agree well with recent neutron PDF results but not with some earlier results. We discuss the limitations of assuming a two peak distribution in view of the two distortions needed to describe the Mn-O distortions as a function of T and B for B≥2T . It is likely that there is a distribution of longer bonds. Finally we show that with increasing B field, the Mn-Mn peak also has a small B -field-induced change—a measure at the unit cell level of magnetostriction but find that there is no observable B -field-induced change in the Mn

  16. 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.

  17. 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.

  18. Photochromism and polaronic photocharge localization in diluted KTa1-xNbxO3

    NASA Astrophysics Data System (ADS)

    Gubaev, A. I.; Kapphan, S. E.; Jastrabik, L.; Trepakov, V. A.; Syrnikov, P. P.

    2006-07-01

    Ultraviolet (UV)-light-induced optical absorption in the near infrared (NIR) region was observed in diluted KTa1-xNbxO3 single crystals (x =0,0.004,0.007,0.012,0.07) at low temperatures. Illumination by wideband light (3.10-4.13eV, 300-400nm) is accompanied by the appearance of a broad NIR absorption band with the position of the maxima varying in the 0.69-0.8eV (1.54-1.79μ, T =1.3K) region for different Nb concentrations. This UV-light-induced absorption is absent in nominally pure KTaO3, as well as in all Nb diluted specimens at elevated temperatures. The centers responsible for the photochromic NIR absorption bands are tied to interband optical transitions of pair Nb4+ electronic polarons. The photochromic experimental data, supplemented by luminescence studies in the visible range, evidence the strong localization of the photocharge carriers by pair Nb4+ polarons at low temperatures. It is suggested that namely the strong localization of the photocarriers plays a crucial role in photoinduced gigantic dielectric effects and possible phase transitions, which have been recognized recently in incipient ferroelectrics at low temperatures.

  19. 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.

  20. 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.

  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 effects on the dc- and ac-tunneling characteristics of molecular Josephson junctions

    NASA Astrophysics Data System (ADS)

    Wu, B. H.; Cao, J. C.; Timm, C.

    2012-07-01

    We study the interplay of polaronic effect and superconductivity in transport through molecular Josephson junctions. The tunneling rates of electrons are dominated by vibronic replicas of the superconducting gap, which show up as prominent features in the differential conductance for the dc and ac current. For relatively large molecule-lead coupling, a features that appears when the Josephson frequency matches the vibron frequency can be identified with an over-the-gap structure observed by Marchenkov [Nat. Nanotech. 1748-338710.1038/nnano.2007.2182, 481 (2007)]. However, we are more concerned with the weak-coupling limit, where resonant tunneling through the molecular level dominates. We find that certain features involving both Andreev reflection and vibron emission show an unusual shift of the bias voltage V at their maximum with the gate voltage Vg as V˜(2/3)Vg. Moreover, due to the polaronic effect, the ac Josephson current shows a phase shift of π when the bias eV is increased by one vibronic energy quantum ℏωv. This distinctive even-odd effect is explained in terms of the different sign of the coupling to vibrons of electrons and of Andreev-reflected holes.

  3. Degradation of wide band-gap electrolumienscent materials by exciton-polaron interactions (Presentation Recording)

    NASA Astrophysics Data System (ADS)

    Aziz, Hany; Wang, Qi

    2015-10-01

    The limited performance stability and gradual loss in the electroluminescence efficiency of OLEDs utilizing wide band-gap materials, such as blue-emitting phosphorescent and fluorescent devices, continues to be a challenge for wider technology adoption. We recently found that interactions between excitons and polarons play an important role in the aging behavior of electroluminescent materials, and that a correlation exists between the susceptibility of these materials to this aging mode and their band-gap. This degradation mode is also found to be often associated with the emergence of new bands - at longer wavelength - in the electroluminescence spectra of the materials, that can often be detected after prolonged electrical driving. Such bands contribute to the increased spectral broadening and color purity loss often observed in these devices over time. Exciton-polaron interactions, and the associated degradation, are also found to occur most significantly in the vicinity of device inter-layer interfaces such as at the interface between the emitter layer and the electron or hole transport layers. New results obtained from investigations of these phenomena in a wide range of commonly used host and guest OLED materials will be presented.

  4. Surface of active polarons: A semiexplicit solvation method for biomolecular dynamics

    NASA Astrophysics Data System (ADS)

    Kimura, S. Roy; Brower, Richard C.; Zhang, Chao; Sugimori, Masamichi

    2000-05-01

    We present a strategy for solvating biomolecules in molecular dynamics or Monte Carlo simulations. The method employs a thin layer (often monomolecular) of explicit water with additional external forces representing the electrostatics, pressure, fluctuations, and dissipations caused by the neglected bulk. Long-range electrostatic corrections are supplied through a set of variable surface charges (polarons) that recreates the mean reaction field (or dielectric properties) of an infinite solvent. We refer to this "fictitious" boundary layer as a "surface of active polarons" (or SOAP). Test simulations of the solvation free energies of 15 amino acid analogs and nine ions are in good agreement with experiment (correlation coefficients: 0.995 and 1.000, respectively) despite the use of unaltered published force-fields with only one adjustable parameter. Dynamical capabilities of SOAP are illustrated by application to a six residue peptide with a stable conformation (SYPFDV), as well as a flexible nine residue HIV-1 gp120 peptide (TLTSCNTSV from PDB 1hhg). Future extensions, calibrations, and applications are discussed briefly.

  5. 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.

  6. Evidence for transition from polaron to bipolaron conduction in electroactive Li{sub x}Cr{sub 0.11}V{sub 2}O{sub 5.16} powders: A dynamic study from 10 to 10{sup 10} Hz

    SciTech Connect

    Badot, J.C.; Dubrunfaut, O.

    2011-12-15

    This paper presents a study on the electrical transport properties of lithiated Cr{sub 0.11}V{sub 2}O{sub 5.16}, which can be used as a rechargeable cathodic material in lithium batteries. Dielectric and conductivity spectra of Li{sub x}Cr{sub 0.11}V{sub 2}O{sub 5.16} powders (x=0, 0.05, 0.40 and 1.20) were recorded in a broad frequency range of 10-10{sup 10} Hz at temperature varying between 300 and 400 K. Complex resistivity diagrams have enabled to obtain thermal behaviors of bulk dc-conductivity. Dielectric relaxations were found, attributed to small polarons and (intersite) bipolarons hopping. The transport properties are shown to be consistent with small polaron and bipolaron conduction models. The change from polaronic to bipolaronic conduction has been evidenced with the increase of the lithium content x from 0.40 to 1.20. This work opens up new prospects for a more fundamental understanding of the electronic transport in relation with the electrochemical properties of Cr{sub 0.11}V{sub 2}O{sub 5.16}. - Graphical Abstract: Schematic structure of Cr{sub 0.11}V{sub 2}O{sub 5.16}. Highlights: Black-Right-Pointing-Pointer Chromium-vanadium mixed oxide as cathodic material. Black-Right-Pointing-Pointer Broadband dielectric spectroscopy from low frequencies to microwaves. Black-Right-Pointing-Pointer Transition from polaron to bipolaron conduction as lithium content increases.

  7. Polaronic effects in manganese oxides: Self-trapped electronic states in lanthanum manganate and sodium chloride

    NASA Astrophysics Data System (ADS)

    Perebeinos, Vasili

    2001-12-01

    Self-trapped states occur in many insulating solids but are not especially well-understood. There is a need for better theoretical models and better experimental tools for exploring these states. This thesis provides models for two kinds of materials LaMnO3 and NaCl, and predicts experimental effects which can be used to characterize such states. LaMnO3 is an insulating antiferromagnet which can be doped with holes over a wide concentration range, as in La1- xCaxMnO3. Here I study the regime x << 1 where particularly interesting and simple behavior is predicted. The model has electronic and lattice-vibrational degrees of freedom chosen to represent the Mn ion outer electronic states and their interaction with oxygen motions in the three dimensional perovskite crystal structure. Four independent types of data are available to choose three adjusted parameters. Using electronic structure calculations, optical conductivity and Raman spectra for this choice the predicted magnitude of the static Jahn-Teller distortion agrees within 10-15% with neutron diffraction data. I use the model to analyze and predict the self-localized states which form under optical excitation and under hole doping. In particular five types of behavior are analyzed: (1)the insulating nature of lightly doped LaMnO3 due to the anti-Jahn-Teller polaron formation; (2)phonon broadening due to the exciton formation; (3)polaronic angle-resolved- photoemission-spectra (ARPES); (4)Raman spectra due to the Franck-Condon mechanism; (5)the self-trapped exciton in NaCl and its optical properties including the Franck-Condon effect using the first-principles Density Functional Theory (DFT) calculations. Experimental confirmation of the predicted behavior for LaMnO3 will differentiate the Jahn-Teller model studied here from competing versions. The results given here are novel in five ways. (1)Essentially exact analytical polaronic spectra of the two-orbital model Hamiltonian have been obtained. (2)Self

  8. Multivalency and polaronic hole trapping in BaBiO3

    NASA Astrophysics Data System (ADS)

    Franchini, Cesare

    2010-03-01

    The phase diagrams of hole-doped oxides have been one of the central issues of condensed-matter physics in the last 20 years. Whereas transition metal oxides are now fairly well understood, the physics of the conceivably ``simpler'' sp bonded oxides is less clear. How is it possible that some of these oxides remain insulating upon doping? By adopting hybrid density functional theory and self-consistent GW we show that the multivalency of the metal cations and the formation of polaronic lattice distortions (i.e the coupling between holes/electrons trapping on specific lattice sites and the accompanying polarization field) can explain this puzzling experimental observation. The example we have chosen is BaBiO3, which remains an insulator upon moderate hole doping and undergoes an insulator to superconductor transition around a hole concentration of 0.35. Pure BaBiO3 is characterized by a charge disproportionation (CD) with half of the Bi atoms possessing a valence 3+ and half a valence 5+. The CD goes in hand with significant structural and electronic changes from the ideal metallic cubic perovskite crystal (BaBi^4+O3) towards an insulating monoclinic structure (Ba2Bi^3+Bi^5+O6) characterized by a charge density wave state formed by alternating breathing-in/out distortions of oxygen octahedra around inequivalent Bi^5+/Bi^3+ ions [1]. Our results show that upon-hole doping Bi^3+ sites trap two holes from the valence band to form Bi^5+ cations, and that the trapping is accompanied by a distortion of the oxygen polarization field that surround the BiO6 octahedra. We show that the strong interaction between polarons ultimately causes an overlap between the polaronic band and the valence band resulting in a metallic non-disproportionated state [2]. [4pt] [1] C. Franchini, A. Sanna, M. Marsman & G. Kresse, arXiv:0803.0619v2 (2009).[0pt] [2] C. Franchini, G. Kresse & R. Podloucky, PRL 102, 256402 (2009).

  9. 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.

  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. 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.

  12. Polaron-molecule transitions in a two-dimensional Fermi gas

    SciTech Connect

    Parish, Meera M.

    2011-05-15

    We address the problem of a single 'spin-down' impurity atom interacting attractively with a spin-up Fermi gas in two dimensions (2D). We consider the case where the mass of the impurity is greater than or equal to the mass of a spin-up fermion. Using a variational approach, we resolve the questions raised by previous studies and show that there is, in fact, a transition between polaron and molecule (dimer) ground states in 2D. For the molecule state, we use a variational wave function with a single particle-hole excitation on the Fermi sea and we find that its energy matches that of the exact solution in the limit of infinite impurity mass. Thus, we expect the variational approach to provide a reliable tool for investigating 2D systems.

  13. Single-polaron properties for double-well electron-phonon coupling

    NASA Astrophysics Data System (ADS)

    Adolphs, Clemens; Berciu, Mona

    2014-03-01

    We introduce a new model to describe electron-phonon coupling in systems such as one-dimensional intercalated chains or two-dimensional CuO2 planes, where symmetry dictates that the linear coupling term vanishes. We show that, under certain conditions, an additional charge carrier dynamically changes the local lattice potential from a harmonic well into a double well. We use the Momentum Average approximation to study the properties of this model in the single-polaron limit. A detailed analysis reveals that despite some qualitative similarities to the linear Holstein model, a renormalized Holstein model cannot account for all of the physics of the double-well model. We thank NSERC and QMI for financial support.

  14. Photoinduced dynamics in doped Mott insulators with polaronic conduction: Ba2Ti13O22 and BaxTi8O16

    NASA Astrophysics Data System (ADS)

    Yamaguchi, N.; Furuhashi, A.; Nishihara, H.; Murata, R.; Takayama, K.; Katsufuji, T.

    2016-07-01

    To clarify the dynamics of polarons in doped Mott insulators, we performed pump-probe reflectivity measurements for two barium titanates, Ba2Ti13O22 and BaxTi8O16 , with a noninteger average number of d electrons per Ti. We found that the photoinduced dynamics in Ba2Ti13O22 with a three-dimensional electronic structure is characterized by a broadening of the polaron-excitation peak immediately after photoirradiation, whereas that in BaxTi8O16 with a one-dimensional electronic structure is characterized by a change in the intensities of the polaron-excitation peak and charge-gap-excitation peak with time. This indicates that a difference in dimensionality results in different photoinduced dynamics of polarons in doped Mott insulators.

  15. 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

  16. Excitons in a photosynthetic light-harvesting system: A combined molecular dynamics, quantum chemistry, and polaron model study

    NASA Astrophysics Data System (ADS)

    Damjanović, Ana; Kosztin, Ioan; Kleinekathöfer, Ulrich; Schulten, Klaus

    2002-03-01

    The dynamics of pigment-pigment and pigment-protein interactions in light-harvesting complexes is studied with an approach that combines molecular dynamics simulations with quantum chemistry calculations and a polaron model analysis. The molecular dynamics simulation of light-harvesting (LH) complexes was performed on an 87 055 atom system comprised of a LH-II complex of Rhodospirillum molischianum embedded in a lipid bilayer and surrounded with appropriate water layers. For each of the 16 B850 bacteriochlorophylls (BChls), we performed 400 ab initio quantum chemistry calculations on geometries that emerged from the molecular dynamical simulations, determining the fluctuations of pigment excitation energies as a function of time. From the results of these calculations we construct a time-dependent Hamiltonian of the B850 exciton system from which we determine within linear response theory the absorption spectrum. Finally, a polaron model is introduced to describe both the excitonic and coupled phonon degrees of freedom by quantum mechanics. The exciton-phonon coupling that enters into the polaron model, and the corresponding phonon spectral function, are derived from the molecular dynamics and quantum chemistry simulations. The model predicts that excitons in the B850 BChl ring are delocalized over five pigments at room temperature. Also, the polaron model permits the calculation of the absorption and circular dichroism spectra of the B850 excitons from the sole knowledge of the autocorrelation function of the excitation energies of individual BChls, which is readily available from the combined molecular dynamics and quantum chemistry simulations. The obtained results are found to be in good agreement with the experimentally measured absorption and circular dichroism spectra.

  17. New insights on the nature of two-dimensional polarons in semiconducting polymers: Infrared absorption in poly(3-hexylthiophene)

    SciTech Connect

    Pochas, Christopher M.; Spano, Frank C.

    2014-06-28

    Infrared absorption of positively charged polarons in conjugated polymer chains and π-stacked aggregates is investigated theoretically, employing a Holstein-based Hamiltonian which treats electronic coupling, electron-vibrational coupling, and disorder on equal footing. The spectra evaluated from the Hamiltonian expressed in a one- and two-particle basis set are essentially exact, insofar as the main, aromatic-quinoidal vibrational mode is treated fully nonadiabatically. Diagonal and off-diagonal (“paracrystalline”) disorder are resolved along the polymer axis (x) and the aggregate stacking axis (y). Disorder along the polymer axis selectively attenuates the x-polarized spectrum, which is dominated by the polaron peak P{sub 1}. Disorder along the stacking axis selectively attenuates the y-polarized spectrum, which is dominated by the lower-energy charge-transfer peak, DP{sub 1}. Calculated spectra are in excellent agreement with the measured induced-absorption and charge-modulation spectra, reproducing the peak positions and relative peak intensities within a line shape rich in vibronic structure. Our nonadiabatic approach predicts the existence of a weak, x-polarized peak P{sub 0}, slightly blueshifted from DP{sub 1}. The peak is intrinsic to single polymer chains and appears in a region of the spectrum where narrow infrared active vibrational modes have been observed in nonaggregated conjugated polymers. The polaron responsible for P{sub 0} is composed mainly of two-particle wave functions and cannot be accounted for in the more conventional adiabatic treatments.

  18. Possible magnetic-polaron-switched positive and negative magnetoresistance in the GdSi single crystals.

    PubMed

    Li, Haifeng; Xiao, Yinguo; Schmitz, Berthold; Persson, Jörg; Schmidt, Wolfgang; Meuffels, Paul; Roth, Georg; Brückel, Thomas

    2012-01-01

    Magnetoresistance (MR) has attracted tremendous attention for possible technological applications. Understanding the role of magnetism in manipulating MR may in turn steer the searching for new applicable MR materials. Here we show that antiferromagnetic (AFM) GdSi metal displays an anisotropic positive MR value (PMRV), up to ~415%, accompanied by a large negative thermal volume expansion (NTVE). Around T(N) the PMRV translates to negative, down to ~-10.5%. Their theory-breaking magnetic-field dependencies [PMRV: dominantly linear; negative MR value (NMRV): quadratic] and the unusual NTVE indicate that PMRV is induced by the formation of magnetic polarons in 5d bands, whereas NMRV is possibly due to abated electron-spin scattering resulting from magnetic-field-aligned local 4f spins. Our results may open up a new avenue of searching for giant MR materials by suppressing the AFM transition temperature, opposite the case in manganites, and provide a promising approach to novel magnetic and electric devices. PMID:23087815

  19. Possible magnetic-polaron-switched positive and negative magnetoresistance in the GdSi single crystals

    PubMed Central

    Li, Haifeng; Xiao, Yinguo; Schmitz, Berthold; Persson, Jörg; Schmidt, Wolfgang; Meuffels, Paul; Roth, Georg; Brückel, Thomas

    2012-01-01

    Magnetoresistance (MR) has attracted tremendous attention for possible technological applications. Understanding the role of magnetism in manipulating MR may in turn steer the searching for new applicable MR materials. Here we show that antiferromagnetic (AFM) GdSi metal displays an anisotropic positive MR value (PMRV), up to ~415%, accompanied by a large negative thermal volume expansion (NTVE). Around TN the PMRV translates to negative, down to ~−10.5%. Their theory-breaking magnetic-field dependencies [PMRV: dominantly linear; negative MR value (NMRV): quadratic] and the unusual NTVE indicate that PMRV is induced by the formation of magnetic polarons in 5d bands, whereas NMRV is possibly due to abated electron-spin scattering resulting from magnetic-field-aligned local 4f spins. Our results may open up a new avenue of searching for giant MR materials by suppressing the AFM transition temperature, opposite the case in manganites, and provide a promising approach to novel magnetic and electric devices. PMID:23087815

  20. Effects of polarons on static polarizabilities and second order hyperpolarizabilities of conjugated polymers

    NASA Astrophysics Data System (ADS)

    Wang, Ya-Dong; Meng, Yan; Di, Bing; Wang, Shu-Ling; An, Zhong

    2010-12-01

    According to the one-dimensional tight-binding Su—Schrieffer—Heeger model, we have investigated the effects of charged polarons on the static polarizability, αxx, and the second order hyperpolarizabilities, γxxxx, of conjugated polymers. Our results are consistent qualitatively with previous ab initio and semi-empirical calculations. The origin of the universal growth is discussed using a local-view formalism that is based on the local atomic charge derivatives. Furthermore, combining the Su-Schrieffer-Heeger model and the extended Hubbard model, we have investigated systematically the effects of electron-electron interactions on αxx and γxxxx of charged polymer chains. For a fixed value of the nearest-neighbour interaction V, the values of αxx and γxxxx increase as the on-site Coulomb interaction U increases for U < Uc and decrease with U for U > Uc, where Uc is a critical value of U at which the static polarizability or the second order hyperpolarizability reaches a maximal value of αmax or γmax. It is found that the effect of the e-e interaction on the value of αxx is dependent on the ratio between U and V for either a short or a long charged polymer. Whereas, that effect on the value of γxxxx is sensitive both to the ratio of U to V and to the size of the molecule.

  1. Polaronic metal state at the LaAlO3/SrTiO3 interface.

    PubMed

    Cancellieri, C; Mishchenko, A S; Aschauer, U; Filippetti, A; Faber, C; Barišić, O S; Rogalev, V A; Schmitt, T; Nagaosa, N; Strocov, V N

    2016-01-01

    Interplay of spin, charge, orbital and lattice degrees of freedom in oxide heterostructures results in a plethora of fascinating properties, which can be exploited in new generations of electronic devices with enhanced functionalities. The paradigm example is the interface between the two band insulators LaAlO3 and SrTiO3 that hosts a two-dimensional electron system. Apart from the mobile charge carriers, this system exhibits a range of intriguing properties such as field effect, superconductivity and ferromagnetism, whose fundamental origins are still debated. Here we use soft-X-ray angle-resolved photoelectron spectroscopy to penetrate through the LaAlO3 overlayer and access charge carriers at the buried interface. The experimental spectral function directly identifies the interface charge carriers as large polarons, emerging from coupling of charge and lattice degrees of freedom, and involving two phonons of different energy and thermal activity. This phenomenon fundamentally limits the carrier mobility and explains its puzzling drop at high temperatures. PMID:26813124

  2. Polaron effects on the performance of light-harvesting systems: a quantum heat engine perspective

    NASA Astrophysics Data System (ADS)

    Xu, Dazhi; Wang, Chen; Zhao, Yang; Cao, Jianshu

    2016-02-01

    We explore energy transfer in a generic three-level system, which is coupled to three non-equilibrium baths. Built on the concept of quantum heat engine, our three-level model describes non-equilibrium quantum processes including light-harvesting energy transfer, nano-scale heat transfer, photo-induced isomerization, and photovoltaics in double quantum-dots. In the context of light-harvesting, the excitation energy is first pumped up by sunlight, then is transferred via two excited states which are coupled to a phonon bath, and finally decays to the reaction center. The efficiency of this process is evaluated by steady state analysis via a polaron-transformed master equation; thus the entire range of the system-phonon coupling strength can be covered. We show that the coupling with the phonon bath not only modifies the steady state, resulting in population inversion, but also introduces a finite steady state coherence which optimizes the energy transfer flux and efficiency. In the strong coupling limit, the steady state coherence disappears and the efficiency recovers the heat engine limit given by Scovil and Schultz-Dubois (1959 Phys. Rev. Lett. 2 262).

  3. 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.

  4. Polaronic metal state at the LaAlO3/SrTiO3 interface

    NASA Astrophysics Data System (ADS)

    Cancellieri, C.; Mishchenko, A. S.; Aschauer, U.; Filippetti, A.; Faber, C.; Barišić, O. S.; Rogalev, V. A.; Schmitt, T.; Nagaosa, N.; Strocov, V. N.

    2016-01-01

    Interplay of spin, charge, orbital and lattice degrees of freedom in oxide heterostructures results in a plethora of fascinating properties, which can be exploited in new generations of electronic devices with enhanced functionalities. The paradigm example is the interface between the two band insulators LaAlO3 and SrTiO3 that hosts a two-dimensional electron system. Apart from the mobile charge carriers, this system exhibits a range of intriguing properties such as field effect, superconductivity and ferromagnetism, whose fundamental origins are still debated. Here we use soft-X-ray angle-resolved photoelectron spectroscopy to penetrate through the LaAlO3 overlayer and access charge carriers at the buried interface. The experimental spectral function directly identifies the interface charge carriers as large polarons, emerging from coupling of charge and lattice degrees of freedom, and involving two phonons of different energy and thermal activity. This phenomenon fundamentally limits the carrier mobility and explains its puzzling drop at high temperatures.

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

    DOE PAGESBeta

    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

  6. Polaronic metal state at the LaAlO3/SrTiO3 interface

    PubMed Central

    Cancellieri, C.; Mishchenko, A. S.; Aschauer, U.; Filippetti, A.; Faber, C.; Barišić, O. S.; Rogalev, V. A.; Schmitt, T.; Nagaosa, N.; Strocov, V. N.

    2016-01-01

    Interplay of spin, charge, orbital and lattice degrees of freedom in oxide heterostructures results in a plethora of fascinating properties, which can be exploited in new generations of electronic devices with enhanced functionalities. The paradigm example is the interface between the two band insulators LaAlO3 and SrTiO3 that hosts a two-dimensional electron system. Apart from the mobile charge carriers, this system exhibits a range of intriguing properties such as field effect, superconductivity and ferromagnetism, whose fundamental origins are still debated. Here we use soft-X-ray angle-resolved photoelectron spectroscopy to penetrate through the LaAlO3 overlayer and access charge carriers at the buried interface. The experimental spectral function directly identifies the interface charge carriers as large polarons, emerging from coupling of charge and lattice degrees of freedom, and involving two phonons of different energy and thermal activity. This phenomenon fundamentally limits the carrier mobility and explains its puzzling drop at high temperatures. PMID:26813124

  7. Observation of a two-dimensional liquid of Fröhlich polarons at the bare SrTiO3 surface

    PubMed Central

    Chen, Chaoyu; Avila, José; Frantzeskakis, Emmanouil; Levy, Anna; Asensio, Maria C.

    2015-01-01

    The polaron is a quasi-particle formed by a conduction electron (or hole) together with its self-induced polarization in a polar semiconductor or an ionic crystal. Among various polarizable examples of complex oxides, strontium titanate (SrTiO3) is one of the most studied. Here we examine the carrier type and the interplay of inner degrees of freedom (for example, charge, lattice, orbital) in SrTiO3. We report the experimental observation of Fröhlich polarons, or large polarons, at the bare SrTiO3 surface prepared by vacuum annealing. Systematic analyses of angle-resolved photoemission spectroscopy and X-ray absorption spectra show that these Fröhlich polarons are two-dimensional and only exist with inversion symmetry breaking by two-dimensional oxygen vacancies. Our discovery provides a rare solvable field theoretical model, and suggests the relevance of large (bi)polarons for superconductivity in perovskite oxides, as well as in high-temperature superconductors. PMID:26489376

  8. Observation of a two-dimensional liquid of Fröhlich polarons at the bare SrTiO3 surface.

    PubMed

    Chen, Chaoyu; Avila, José; Frantzeskakis, Emmanouil; Levy, Anna; Asensio, Maria C

    2015-01-01

    The polaron is a quasi-particle formed by a conduction electron (or hole) together with its self-induced polarization in a polar semiconductor or an ionic crystal. Among various polarizable examples of complex oxides, strontium titanate (SrTiO3) is one of the most studied. Here we examine the carrier type and the interplay of inner degrees of freedom (for example, charge, lattice, orbital) in SrTiO3. We report the experimental observation of Fröhlich polarons, or large polarons, at the bare SrTiO3 surface prepared by vacuum annealing. Systematic analyses of angle-resolved photoemission spectroscopy and X-ray absorption spectra show that these Fröhlich polarons are two-dimensional and only exist with inversion symmetry breaking by two-dimensional oxygen vacancies. Our discovery provides a rare solvable field theoretical model, and suggests the relevance of large (bi)polarons for superconductivity in perovskite oxides, as well as in high-temperature superconductors. PMID:26489376

  9. Observation of a two-dimensional liquid of Fröhlich polarons at the bare SrTiO3 surface

    NASA Astrophysics Data System (ADS)

    Chen, Chaoyu; Avila, José; Frantzeskakis, Emmanouil; Levy, Anna; Asensio, Maria C.

    2015-10-01

    The polaron is a quasi-particle formed by a conduction electron (or hole) together with its self-induced polarization in a polar semiconductor or an ionic crystal. Among various polarizable examples of complex oxides, strontium titanate (SrTiO3) is one of the most studied. Here we examine the carrier type and the interplay of inner degrees of freedom (for example, charge, lattice, orbital) in SrTiO3. We report the experimental observation of Fröhlich polarons, or large polarons, at the bare SrTiO3 surface prepared by vacuum annealing. Systematic analyses of angle-resolved photoemission spectroscopy and X-ray absorption spectra show that these Fröhlich polarons are two-dimensional and only exist with inversion symmetry breaking by two-dimensional oxygen vacancies. Our discovery provides a rare solvable field theoretical model, and suggests the relevance of large (bi)polarons for superconductivity in perovskite oxides, as well as in high-temperature superconductors.

  10. Hybrid functional study of the NASICON-type Na3V2(PO4)3: crystal and electronic structures, and polaron-Na vacancy complex diffusion.

    PubMed

    Bui, Kieu My; Dinh, Van An; Okada, Susumu; Ohno, Takahisa

    2015-11-11

    The crystal and electronic structures, electrochemical properties and diffusion mechanism of NASICON-type Na3V2(PO4)3 have been investigated based on the hybrid density functional Heyd-Scuseria-Ernzerhof (HSE06). A polaron-Na vacancy complex model for revealing the diffusion mechanism is proposed for the first time in the field of Na-ion batteries. The bound polaron is found to favorably form at the first nearest V site to the Na vacancy. Consequently, the movement of the Na vacancy will be accompanied by the polaron. Three preferable diffusion pathways are revealed; these are two intra-layer diffusion pathways and one inter-layer pathway. The activation barriers for the intra-layer and inter-layer pathways are 353 meV and 513 meV, respectively. For further comparison, the generalized gradient approximation with an onsite Coulomb Hubbard U (GGA+U) is also employed. PMID:26509737

  11. Exploring the impact of semicore level electronic relaxation on polaron dynamics: An adiabatic ab initio study of FePO4

    NASA Astrophysics Data System (ADS)

    Wang, Zi; Bevan, Kirk H.

    2016-01-01

    In the present work, we study the effects of the electronic relaxation of semicore levels on polaron activation energies and dynamics. Within the framework of adiabatic ab initio theory, we utilize both static transition state theory and molecular dynamics methods for an in-depth study of polaronic hopping in delithiated LiFePO4 (FePO4). Our results show that electronic relaxation of semicore states is significant in FePO4, resulting in a lower activation barrier and kinetics that is one to two orders faster compared to the result of calculations that do not incorporate semicore states. In general, the results suggest that the relaxation of states far below the Fermi energy could dramatically impact the ab initio polaronic barrier estimates for many transition metal oxides and phosphates.

  12. Angle-resolved photoemission spectroscopy of the insulating NaxWO3: Anderson localization, polaron formation, and remnant Fermi surface.

    PubMed

    Raj, S; Hashimoto, D; Matsui, H; Souma, S; Sato, T; Takahashi, T; Sarma, D D; Mahadevan, Priya; Oishi, S

    2006-04-14

    The electronic structure of the insulating sodium tungsten bronze, Na(0.025)WO(3), is investigated by high-resolution angle-resolved photoemission spectroscopy. We find that near-E(F) states are localized due to the strong disorder arising from random distribution of Na+ ions in the WO(3) lattice, which makes the system insulating. The temperature dependence of photoemission spectra provides direct evidence for polaron formation. The remnant Fermi surface of the insulator is found to be the replica of the real Fermi surface in the metallic system. PMID:16712121

  13. Bi-stability in single impurity Anderson model with strong electron-phonon interaction(polaron regime)

    NASA Astrophysics Data System (ADS)

    Eskandari-asl, Amir

    2016-09-01

    We consider a single impurity Anderson model (SIAM) in which the quantum dot(QD) is strongly coupled to a phonon bath in polaron regime. This coupling results in an effective e-e attraction. By computing the self energies using a current conserving approximation which is up to second order in this effective attraction, we show that if the interaction is strong enough, in non particle-hole (PH) symmetric case, the system would be bi-stable and we have hysteresis loop in the I-V characteristic. Moreover, the system shows negative differential conductance in some bias voltage intervals.

  14. Effective Landé factor in a GaMnAs quantum dot; with the effects of sp-d exchange on a bound polaron

    SciTech Connect

    Lalitha, D. Peter, A. John

    2014-04-24

    The effective g-factor of conduction (valence) band electron (hole) is obtained in the GaMnAs quantum dot. Magneto bound polaron in a GaMnAs/Ga{sub 0.6}Al{sub 0.4}As quantum dot is investigated with the inclusion of exchange interaction effects due to Mn alloy content and the geometrical confinement. The spin polaronic energy of the heavy hole exciton is studied with the spatial confinement using a mean field theory in the presence of magnetic field strength.

  15. Effective Landé factor in a GaMnAs quantum dot; with the effects of sp-d exchange on a bound polaron

    NASA Astrophysics Data System (ADS)

    Lalitha, D.; Peter, A. John

    2014-04-01

    The effective g-factor of conduction (valence) band electron (hole) is obtained in the GaMnAs quantum dot. Magneto bound polaron in a GaMnAs/Ga0.6Al0.4As quantum dot is investigated with the inclusion of exchange interaction effects due to Mn alloy content and the geometrical confinement. The spin polaronic energy of the heavy hole exciton is studied with the spatial confinement using a mean field theory in the presence of magnetic field strength.

  16. Electron and hole polaron accumulation in low-bandgap ambipolar donor-acceptor polymer transistors imaged by infrared microscopy

    NASA Astrophysics Data System (ADS)

    Khatib, O.; Mueller, A. S.; Stinson, H. T.; Yuen, J. D.; Heeger, A. J.; Basov, D. N.

    2014-12-01

    A resurgence in the use of the donor-acceptor approach in synthesizing conjugated polymers has resulted in a family of high-mobility ambipolar systems with exceptionally narrow energy bandgaps below 1 eV. The ability to transport both electrons and holes is critical for device applications such as organic light-emitting diodes and transistors. Infrared spectroscopy offers direct access to the low-energy excitations associated with injected charge carriers. Here we use a diffraction-limited IR microscope to probe the spectroscopic signatures of electron and hole injection in the conduction channel of an organic field-effect transistor based on an ambipolar DA polymer polydiketopyrrolopyrrole-benzobisthiadiazole. We observe distinct polaronic absorptions for both electrons and holes and spatially map the carrier distribution from the source to drain electrodes for both unipolar and ambipolar biasing regimes. For ambipolar device configurations, we observe the spatial evolution of hole-induced to electron-induced polaron absorptions throughout the transport path. Our work provides a platform for combined transport and infrared studies of organic semiconductors on micron length scales relevant to functional devices.

  17. Role of polaron hopping in leakage current behavior of a SrTiO{sub 3} single crystal

    SciTech Connect

    Cao, Y. Randall, C. A.; Chen, L. Q.; Bhattacharya, S.; Shen, J.

    2013-12-14

    We studied the ionic/electronic transport and resistance degradation behavior of dielectric oxides by solving the electrochemical transport equations. Here, we took into account the non-periodical boundary conditions for the transport equations using the Chebyshev collocation algorithm. A sandwiched Ni|SrTiO{sub 3}|Ni capacitor is considered as an example under the condition of 1.0 V, 1.0 μm thickness for SrTiO{sub 3} layer, and a temperature of 150 °C. The applied voltage resulted in the migration of ionic defects (oxygen vacancies) from anode towards cathode. The simulated electric potential profile at steady state is in good agreement with the recent experimental observation. We introduced the possibility of polaron-hopping between Ti{sup 3+} and Ti{sup 4+} at the electrode interface. It is shown that both the oxygen vacancy transport and the polaron-hopping contribute to the resistance degradation of single crystal SrTiO{sub 3}, which is consistent with the experimental observations.

  18. Insulator -- polaron conductor -- metal transitions in a complex oxide 12CaO.7Al2O3.

    NASA Astrophysics Data System (ADS)

    Sushko, P.; Shluger, A.; Stoneham, A.; Hayashi, K.; Matsuishi, S.; Hirano, M.; Hosono, H.

    2006-03-01

    Recent experiments have demonstrated that a complex nano-porous oxide 12CaO.7Al2O3 (C12A7) built of positively charged sub-nanometer cages can be converted from a transparent insulator to a transparent conductor by H2 doping followed by UV-light irradiation with 4--4.5 eV photons [1]. This irradiation induces optical absorption bands with maxima at 0.4 eV and 2.8 eV and high concentrations of unpaired electrons. We use ab initio calculations to reveal the mechanism of photo-induced insulator--conductor transition and the role of H atoms in this process and to elucidate the transport properties of the electrons in this system as a function of electron concentration. Our theoretical modeling suggests that at concentration below 10^20 cm-3 electrons are responsible for the polaron type electrical conductivity with the activation energy close to 0.1 eV as well as for the optical absorption at 0.4 eV and 2.8 eV [2]. We demonstrate that, as the electron concentration exceeds 10^20 cm-3, the character of electronic conductivity changes from polaron type to metallic. [1] K. Hayashi et al., Nature 419, 462 (2002). [2] P.V. Sushko, et al., Phys. Rev. Lett. 91, 126401 (2003); P.V. Sushko et al., Appl. Phys. Lett. 86, 092101 (2005).

  19. Anomalous dispersion and band gap reduction in UO2+x and its possible coupling to the coherent polaronic quantum state

    NASA Astrophysics Data System (ADS)

    Conradson, Steven D.; Andersson, David A.; Bagus, Paul S.; Boland, Kevin S.; Bradley, Joseph A.; Byler, Darrin D.; Clark, David L.; Conradson, Dylan R.; Espinosa-Faller, Francisco J.; Lezama Pacheco, Juan S.; Martucci, Mary B.; Nordlund, Dennis; Seidler, Gerald T.; Valdez, James A.

    2016-05-01

    Hypervalent UO2, UO2(+x) formed by both addition of excess O and photoexcitation, exhibits a number of unusual or often unique properties that point to it hosting a polaronic Bose-Einstein(-Mott) condensate. A more thorough analysis of the O X-ray absorption spectra of UO2, U4O9, and U3O7 shows that the anomalous increase in the width of the spectral features assigned to predominantly U 5f and 6d final states that points to increased dispersion of these bands occurs on the low energy side corresponding to the upper edge of the gap bordered by the conduction or upper Hubbard band. The closing of the gap by 1.5 eV is more than twice as much as predicted by calculations, consistent with the dynamical polaron found by structural measurements. In addition to fostering the excitation that is the proposed mechanism for the coherence, the likely mirroring of this effect on the occupied, valence side of the gap below the Fermi level points to increased complexity of the electronic structure that could be associated with the Fermi topology of BEC-BCS crossover and two band superconductivity.

  20. Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport

    SciTech Connect

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

    2015-04-28

    Quantum transport in disordered systems is studied using a polaron-based master equation. The polaron approach is capable of bridging the results from the coherent band-like transport regime governed by the Redfield equation to incoherent hopping transport in the classical regime. A non-monotonic dependence of the diffusion coefficient is observed both as a function of temperature and system-phonon coupling strength. In the band-like transport regime, the diffusion coefficient is shown to be linearly proportional to the system-phonon coupling strength and vanishes at zero coupling due to Anderson localization. In the opposite classical hopping regime, we correctly recover the dynamics described by the Fermi’s Golden Rule and establish that the scaling of the diffusion coefficient depends on the phonon bath relaxation time. In both the hopping and band-like transport regimes, it is demonstrated that at low temperature, the zero-point fluctuations of the bath lead to non-zero transport rates and hence a finite diffusion constant. Application to rubrene and other organic semiconductor materials shows a good agreement with experimental mobility data.

  1. Coherent quantum transport in disordered systems: A unified polaron treatment of hopping and band-like transport.

    PubMed

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

    2015-04-28

    Quantum transport in disordered systems is studied using a polaron-based master equation. The polaron approach is capable of bridging the results from the coherent band-like transport regime governed by the Redfield equation to incoherent hopping transport in the classical regime. A non-monotonic dependence of the diffusion coefficient is observed both as a function of temperature and system-phonon coupling strength. In the band-like transport regime, the diffusion coefficient is shown to be linearly proportional to the system-phonon coupling strength and vanishes at zero coupling due to Anderson localization. In the opposite classical hopping regime, we correctly recover the dynamics described by the Fermi's Golden Rule and establish that the scaling of the diffusion coefficient depends on the phonon bath relaxation time. In both the hopping and band-like transport regimes, it is demonstrated that at low temperature, the zero-point fluctuations of the bath lead to non-zero transport rates and hence a finite diffusion constant. Application to rubrene and other organic semiconductor materials shows a good agreement with experimental mobility data. PMID:25933748

  2. Effect of Förster-mediated triplet-polaron quenching and triplet-triplet annihilation on the efficiency roll-off of organic light-emitting diodes

    NASA Astrophysics Data System (ADS)

    van Eersel, H.; Bobbert, P. A.; Janssen, R. A. J.; Coehoorn, R.

    2016-04-01

    We report the results of a systematic study of the interplay of triplet-polaron quenching (TPQ) and triplet-triplet annihilation (TTA) on the efficiency roll-off of organic light-emitting diodes (OLEDs) with increasing current density. First, we focus on OLEDs based on the green phosphorescent emitter tris[2-phenylpyridine]iridium(III) (Ir(ppy)3) and the red phosphorescent dye platinum octaethylporphyrin. It is found that the experimental data can be reproduced using kinetic Monte Carlo (kMC) simulations within which TPQ and TTA are due to a nearest-neighbor (NN) interaction, or due to a more long-range Förster-type process. Furthermore, we find a subtle interplay between TPQ and TTA: decreasing the contribution of one process can increase the contribution of the other process, so that the roll-off is not significantly reduced. Furthermore, we find that just analyzing the shape of the roll-off is insufficient for determining the relative role of TPQ and TTA. Subsequently, we investigate the wider validity of this picture using kMC simulations for idealized but realistic symmetric OLEDs, with an emissive layer containing a small concentration of phosphorescent dye molecules in a matrix material. Whereas for NN-interactions the roll-off can be reduced when the dye molecules act as shallow hole and electron traps, we find that such an approach becomes counterproductive for long-range TTA and TPQ. Developing well-founded OLED design rules will thus require that more quantitative information is available on the rate and detailed mechanism of the TPQ and TTA processes.

  3. Quasiparticle motion in some classical and quantum mechanical systems: Investigations of nanoscale friction and polaron mobility

    NASA Astrophysics Data System (ADS)

    Tiwari, Mukesh

    -trapping observed in these systems. A review of the derivation of the generalized master equation and the relationship of the memory function to bath spectra is also provided. The formal theory is then applied to the 2-site nondegenerate quantum mechanical polaron model and the effect of a constant electric field on the evolution is studied both in the short and long time limit. The role of temperature and of coupling to the bath on the spectrum, and ultimately on the evolution, are also discussed.

  4. Charge Transport in 4 nm Molecular Wires with Interrupted Conjugation: Combined Experimental and Computational Evidence for Thermally Assisted Polaron Tunneling.

    PubMed

    Taherinia, Davood; Smith, Christopher E; Ghosh, Soumen; Odoh, Samuel O; Balhorn, Luke; Gagliardi, Laura; Cramer, Christopher J; Frisbie, C Daniel

    2016-04-26

    We report the synthesis, transport measurements, and electronic structure of conjugation-broken oligophenyleneimine (CB-OPI 6) molecular wires with lengths of ∼4 nm. The wires were grown from Au surfaces using stepwise aryl imine condensation reactions between 1,4-diaminobenzene and terephthalaldehyde (1,4-benzenedicarbaldehyde). Saturated spacers (conjugation breakers) were introduced into the molecular backbone by replacing the aromatic diamine with trans-1,4-diaminocyclohexane at specific steps during the growth processes. FT-IR and ellipsometry were used to follow the imination reactions on Au surfaces. Surface coverages (∼4 molecules/nm(2)) and electronic structures of the wires were determined by cyclic voltammetry and UV-vis spectroscopy, respectively. The current-voltage (I-V) characteristics of the wires were acquired using conducting probe atomic force microscopy (CP-AFM) in which an Au-coated AFM probe was brought into contact with the wires to form metal-molecule-metal junctions with contact areas of ∼50 nm(2). The low bias resistance increased with the number of saturated spacers, but was not sensitive to the position of the spacer within the wire. Temperature dependent measurements of resistance were consistent with a localized charge (polaron) hopping mechanism in all of the wires. Activation energies were in the range of 0.18-0.26 eV (4.2-6.0 kcal/mol) with the highest belonging to the fully conjugated OPI 6 wire and the lowest to the CB3,5-OPI 6 wire (the wire with two saturated spacers). For the two other wires with a single conjugation breaker, CB3-OPI 6 and CB5-OPI 6, activation energies of 0.20 eV (4.6 kcal/mol) and 0.21 eV (4.8 kcal/mol) were found, respectively. Computational studies using density functional theory confirmed the polaronic nature of charge carriers but predicted that the semiclassical activation energy of hopping should be higher for CB-OPI molecular wires than for the OPI 6 wire. To reconcile the experimental and

  5. Angle-resolved photoemission studies of lattice polaron formation in the cuprate Ca2CuO2Cl2

    SciTech Connect

    Shen, K.M.

    2010-05-03

    To elucidate the nature of the single-particle excitations in the undoped parent cuprates, we have performed a detailed study of Ca{sub 2}CuO{sub 2}Cl{sub 2} using photoemission spectroscopy. The photoemission lineshapes of the lower Hubbard band are found to be well-described by a polaron model. By comparing the lineshape and temperature dependence of the lower Hubbard band with additional O 2p and Ca 3p states, we conclude that the dominant broadening mechanism arises from the interaction between the photohole and the lattice. The strength of this interaction was observed to be strongly anisotropic and may have important implications for the momentum dependence of the first doped hole states.

  6. Temperature dependent electron spin echo studies of polarons in donor- and acceptor-doped poly(p-phenylene): Structural studies

    SciTech Connect

    Kispert, L.D.; Joseph, J.; Tang, J.; Bowman, M.K.; Van Brakel, G.H.; Norris, J.R.

    1986-06-06

    Electron spin echo (ESE) measurements of donor-doped (Li, Na, K and Cs) and acceptor-doped (AsF/sub 5/) poly(p-phenylene), PPP, and fully deuterated PPP samples predict a temperature independent EPR linewidth equal to less than 0.65 gauss that decreases with increasing conductivity. In contrast, EPR linewidths either decrease or increase with decreasing temperature, are dependent on dopant and always exhibit a linewidth either equal to or larger than that predicted from ESE measurements. Deuteration studies indicate that rapid spin exchange is present. Analysis of these results suggest that an exchange exists between isolated radicals in equilibrium with polarons and bipolarons with the equilibrium in favor of bipolarons at 4 K.

  7. Temperature effects on excited state of strong-coupling polaron in an asymmetric RbCl quantum dot

    NASA Astrophysics Data System (ADS)

    Feng, Li-Qin; Li, Jing-Qi; Xiao, Jing-Lin

    2015-01-01

    On the condition of strong electron-LO phonon coupling in an asymmetric RbCl quantum dot (QD), the first excited state energy (FESE), the excitation energy (EE), and the transition frequency (TF) between the first excited ground states (FEGS) of the polaron are calculated by using the linear combination operator and the unitary transformation methods. The variation of the FESE, the EE and the TF with the temperature, the transverse and longitudinal confinement strengths (TLCS) of the QD are studied in detail. We find that the FESE, the EE and the TF decreases (increases) with increasing temperature when the temperature is in lower (higher) temperature regime. They are increasing functions of the TLCS. We find three ways to tune the FESE, the EE and the TF via controlling the temperature and the TLCS.

  8. Formation and diffusion of vacancy-polaron complex in olivine-type LiMnPO4 and LiFePO4

    NASA Astrophysics Data System (ADS)

    Asari, Yusuke; Suwa, Yuji; Hamada, Tomoyuki

    2011-10-01

    Formation and diffusion of a vacancy-polaron complex in olivine-type cathode-active materials, namely, LiMPO4 (M = Fe, Mn), were theoretically investigated by using the first-principles density functional theory within a framework of GGA + U method. It is shown that a lithium vacancy and a corresponding hole-polaron form the complex at the fully lithiated limit owing to lattice distortion and Coulomb interaction between them. It is also shown that the formation energy of the complex in LiMnPO4 is 0.19 eV higher than that in LiFePO4, since a hole polaron in LiMnPO4 is not sufficiently relaxed. As a result, the nucleation rate of MnPO4 phase in LiMnPO4 is 10-3 times slower than that in LiFePO4 and represents the main difference between the kinetics in the initial stage of charging of the two olivine materials. It was also found that the activation energy of the complex diffusion is limited by vacancy hopping in LiMnPO4, while it is determined by both vacancy hopping and polaron hopping in LiFePO4. The activation energy in LiMnPO4, 0.38 eV, is comparable with that in LiFePO4, 0.42 eV. The calculated potential energy profile, showed that the minimum energy path of the diffusing lithium in LiMnPO4 has the same winding shape as that in LiFePO4.

  9. Probing electrons in TiO2 polaronic trap states by IR-absorption: evidence for the existence of hydrogenic states.

    PubMed

    Sezen, Hikmet; Buchholz, Maria; Nefedov, Alexei; Natzeck, Carsten; Heissler, Stefan; Di Valentin, Cristiana; Wöll, Christof

    2014-01-01

    An important step in oxide photochemistry, the loading of electrons into shallow trap states, was studied using infrared (IR) spectroscopy on both, rutile TiO2 powders and single-crystal, r-TiO2(110) oriented samples. After UV-irradiation or n-doping by exposure to H-atoms broad IR absorption lines are observed for the powders at around 940 cm(-1). For the single crystal substrates, the IR absorption bands arising from an excitation of the trapped electrons into higher-lying final states show additional features not observed in previous work. On the basis of our new, high-resolution data and theoretical studies on the polaron binding energy in rutile we propose that the trap states correspond to polarons and are thus intrinsic in nature. We assign the final states probed by the IR-experiments to hydrogenic states within the polaron potential. Implications of these observations for photochemistry on oxides will be briefly discussed. PMID:24448350

  10. 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.