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At least 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2018

Room temperature magnetic ordering and analysis by bound magnetic polaron model of Yb3+ doped nanocrystalline zinc oxide (Zn0.98Yb0.02O)

Highlights: • ZnO and Yb doped ZnO are synthesized by co-precipitation method. • Rietvelt anlysis of XRD patterns confirms the complete substitution of Yb{sup 3+} in ZnO. • Vacancy and defect mediated RTFM is introduced in doped ZnO. • BMP model successfully analyze the magnetic property of Zn{sub 0.98}Yb{sub 0.02}O. - Abstract: Nanocrystalline ZnO and Yb-doped ZnO (Zn{sub 0.98}Yb{sub 0.02}O) are prepared by simple co-precipitation method. The pure crystallographic phases of ZnO and Zn{sub 0.98}Yb{sub 0.02}O are confirmed by Rietveld analyses of XRD patterns. Raman and photoluminescence spectra recorded at room temperature (RT) indicates that lattice defects and oxygen vacancy in Zn{sub 0.98}Yb{sub 0.02}O is more than that of ZnO. Magnetic measurements of ZnO and Zn{sub 0.98}Yb{sub 0.02}O are carried out from 300 to 5 K. Ferromagnetic ordering is observed in Zn{sub 0.98}Yb{sub 0.02}O at RT and the strength of the ordering increases with the lowering of temperature. Ferromagnetism of Zn{sub 0.98}Yb{sub 0.02}O is attributed to the oxygen vacancy introduced by annealing in vacuum. Magnetization vs. temperature curve is well fitted by the combination of 3D spin wave and Curie-Weiss law, which suggest simultaneous presence of para- and ferro-magnetic phases in Zn{sub 0.98}Yb{sub 0.02}O. Ferromagnetic ordering is successfully explained by vacancy mediated bound-magnetic polaron model.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

The Role of Exciton Binding Energy on LO phonon Broadening and Polaron Formation in (BA) 2 PbI 4 Ruddlesden-Popper Films

The effect of carrier–carrier and carrier–phonon interactions is presented in n = 1 (2D) (BA) 2 PbI 4 Ruddlesden–Popper thin films, and their effect is compared to that of conventional MAPbI 3 . While temperature-dependent photoluminescence shows the well-studied structural phase transitions and evidence of longitudinal optical (LO) phonon scattering in MPbI 3 , the 2D (BA) 2 PbI 4 films produce subtler properties. At low temperatures, evidence of two competing intrinsic exciton transitions is observed (P1 and P3), in addition to several extrinsic transitions attributed to the impurities in the (BA) 2 PbI 4 film. At higher temperatures, (BA) 2 PbI 4 is dominated by the two intrinsic excitons that are attributed to varying degrees of localization caused by deformations of the PbI 4 framework mediated by structural relaxation. Although both exciton complexes are well separated from the continuum (490 meV or greater), their interaction with phonons is quite different. In the case of the more strongly bound complex (P3), the strong excitonic nature and short-range interaction are mediated by the emission of LO phonon replicas. In the case of the exciton with the smaller binding energy (P1), the more extended wavefunction manifests itself in strong carrier–phonon scattering and evidence of large, stable polarons.

2D perovskites↗
DOE OSTI2012

Kinetic Monte Carlo Study of Ambipolar Lithium Ion and Electron–Polaron Diffusion into Nanostructured TiO2

Nanostructured titania (TiO2) polymorphs have proved to be promising electrode materials for next generation lithium-ion batteries. However, there is still a lack of understanding of the fundamental microscopic processes that control charge transport in these materials. Here we present microscopic simulations of the collective dynamics of lithium-ion (Li+) and charge compensating electron polarons (e-) in rutile TiO2 nanoparticles in contact with idealized conductive matrix and electrolyte. Kinetic Monte Carlo simulations are used, parameterized by molecular dynamics-based predictions of activation energy barriers for Li+ and e- diffusion. Simulations reveal the central role of electrostatic coupling between Li+ and e- on their collective drift diffusion at the nanoscale. They also demonstrate that high contact area between conductive matrix and rutile nanoparticles leads to undesirable coupling-induced surface saturation effects during Li+ insertion, which limits the overall capacity and conductivity of the material. These results help provide guidelines for design of nanostructured electrode materials with improved electrochemical performance.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2014

High temperature transport properties of thermoelectric CaMnO{sub 3−δ} — Indication of strongly interacting small polarons

The conductivity and Seebeck coefficient of CaMnO{sub 3−δ} have been studied at temperatures up to 1000 °C and in atmospheres with controlled oxygen partial pressure. Both transport coefficients were varied in situ by the reversible formation of oxygen vacancies up to δ = 0.15. The charge carrier concentration was calculated using a defect chemical model. The Seebeck coefficient could be approximated by Heikes' formula, while the conductivity shows a maximum at a molar charge carrier concentration of 0.25. These results were interpreted as a signature of strong electronic correlation effects, and it was concluded that charge transport in CaMnO{sub 3−δ} occurs via strongly interacting small polarons. General prospects for strongly correlated materials as potential candidates for high temperature thermoelectric power generation were discussed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

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

We have investigated dynamics of different localized exciton magnetic polarons (LEMPs) in Cd{sub 0.70}Mn{sub 0.30}Te spin glass (SG) compound below the freezing temperature T{sub f} in the crystal regions, where various microscopic magnetic spin states (MMSSs), namely, “loose” spins, finite, and infinite clusters, are formed. It was shown that there is a broad distribution of the LEMPs lifetimes. The presence of the long-lived LEMPs is caused by the admixture of the optically active bright exciton states to the dark exciton states, i.e., the “brightening” of the dark LEMPs which exist along with the bright LEMPs. The lifetimes of the dark LEMPs correspond to hundreds of nanoseconds. It was found that the time decay of photoluminescence band intensity is approximated by the sum of two functions: a single exponential function and the Kohlrausch–Williams–Watts stretched exponential function. The stretched exponential function describes the recombination processes of the LEMPs formed in the crystal regions of the finite clusters as well as the infinite cluster. This reflects the appearance of spatially heterogeneous dynamics in Cd{sub 0.70}Mn{sub 0.30}Te SG compound below T{sub f} which is due to the disorder in the spin distribution caused by the formation of different MMSSs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Study of spin-polaron formation in 1D systems

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.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Thermodynamics of the polaron master equation at finite bias

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.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2015

Anomalous electrical relaxation and polaron conduction in nano-crystalline Mn{sub 0.5}Zn{sub 0.5}Fe{sub 2}O{sub 4}

Nano-crystalline Mn{sub 0.5}Zn{sub 0.5}Fe{sub 2}O{sub 4} was synthesized by chemical co-precipitation method and characterized with X-ray diffraction. Ac electrical impedance data are taken for the frequency range of 1Hz to 1MHz for various temperatures from 303K to 483K. The ac electrical conduction deviates from the Debye type relaxation which indicates polaron type conduction. In the present study unique anomalous relaxation function in time and frequency domain is used to investigate deviation from the Debye relaxation. The physical basis of anomalous or non-Debye process is explained in terms of change in Debye dipole μ{sub D}=ρr{sub D} of charge ρ into gρ due to the molecular charge interaction and defect disorder. This interaction shifts the Debye relaxation rate τ to a slow relaxation rate τ{sup g}. The fraction 0<g<1 is emerged as the exponent on frequency and time domain function of non-Debye relaxation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

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

Magneto-LO-polaron in a cylindrical GaAs{sub 0.9} P{sub 0.1} / GaAs{sub 0.6} P{sub 0.4} quantum dot is investigated taking into consideration of geometrical confinement effect. The effects of phonon on the exciton binding energy and the interband emission energy as a function of dot radius are found. The calculations are performed within the single band effective mass approximation using the variational method based on the Lee-Low-Pine LLP transformation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Polaron response dominated multiferroic property in 12R-type hexagonal Ba(Ti{sub 1/3}Mn{sub 2/3})O{sub 3-δ} ceramics

We report the multiferroic properties of 12R-type hexagonal Ba(Ti{sub 1/3}Mn{sub 2/3})O{sub 3-δ} found in Mn-doped BaTiO{sub 3} series samples. Hysteresis measurements reveal the coexistence of weak ferromagnetism and ferroelectricity at room temperature. Furthermore, frequency-driven dynamic ferroelectric phase transition is disclosed around a critical frequency of 220 Hz. Analyses on the dielectric relaxation, leakage current, crystal structure, and magnetic susceptibility lead us to conclude that the response of polarons dominates the observed physical properties, and the dynamic phase transition may ascribe to the response mode changes of the localized electrons. More importantly, we figure out the crucial factors leading to difference of the ferroelectric and magnetic properties of the 12R-type Ba(Ti{sub 1/3}Mn{sub 2/3})O{sub 3-δ} samples from that of the 6H-type Ba(Ti{sub 1-x}M{sub x})O{sub 3-δ} (M = Fe, Mn) samples.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

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

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){sub 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.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Donor defects and small polarons on the TiO{sub 2}(110) surface

The role of defects in the chemical activity of the rutile TiO{sub 2}(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 TiO{sub 2} and related oxides.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Photoinduced phase separation in the lead halides is a polaronic effect

We present a perspective on recent observations of the photoinduced phase separation of halides in multi-component lead-halide perovskites. The spontaneous phase separation of an initial homogeneous solid solution under steady-state illumination conditions is found experimentally to be reversible, stochastic, weakly dependent on morphology, yet strongly dependent on composition and thermodynamic state. Regions enriched in a specific halide species that form upon phase separation are self-limiting in size, pinned to specific compositions, and grow in number in proportion to the steady-state carrier concentration until saturation. These empirical observations of robustness rule out explanations based on specific defect structures and point to the local modulation of an existing miscibility phase transition in the presence of excess charge carriers. A model for rationalizing existing observations based on the coupling between composition, strain, and charge density fluctuations through the formation of polarons is reviewed.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

The interplay of excitonic delocalization and vibrational localization in optical lineshapes: A variational polaron approach

The dynamics of molecular excitonic systems are complicated by a competition between electronic coupling (which drives delocalization) and vibrational-electronic (vibronic) interactions (which tend to encourage electronic localization). A particular challenge of molecular systems is that they typically possess a large number of independent vibrations, with frequencies often spanning the entire spectrum of relevant electronic energy gaps. Recent spectroscopic observations and numerical simulations on a water-soluble chlorophyll-binding protein (WSCP) reveal a transition between two regimes of vibronic behavior, a Redfield-like regime in which low-frequency vibrations respond to a delocalized excitonic state, and a Förster-like regime where high-frequency vibrations act as incoherent excitations on individual pigments. Although numerical simulations can reproduce these effects, there is a need for a simple, systematic theory that accurately describes the smooth transition between these two regimes in experimental spectra. Here we address this challenge by generalizing the variational polaron transform approach of [Bloemsma et al., Chem. Phys. 481, 250 (2016)] to include arbitrary bath densities for systems with or without symmetry. We benchmark this theory against both numerical matrix-diagonalization methods and experimental 77 K fluorescence spectra for two WSCP variants, obtaining quite satisfactory agreement in both cases. Here, we apply this theory to offer an explanation for the large loss in apparent electronic coupling in the WSCP Q57K mutant and to examine the likely impact of the interplay between excitonic delocalization and vibrational localization on vibrational sideband shapes and apparent coupling strengths in high-resolution optical spectra for chlorophyll-protein complexes such as WSCP.

14 SOLAR ENERGY↗
DOE OSTI2025

Mixed quantum-classical methods for polaron spectral functions

In this work, using two distinct semiclassical approaches—namely, the mean-field Ehrenfest method and the mapping approach to surface hopping—we investigate the spectral function of a single charge interacting with phonons on a lattice. This quantity is relevant for the description of angle-resolved photoemission experiments. Focusing on the one-dimensional Holstein model, we compare the performance of these approaches across a range of coupling strengths and lattice sizes, exposing the relative strengths and weaknesses of each. We demonstrate that these approaches can be efficiently applied with reasonable accuracy to ab initio polaron models. Furthermore, our work provides a route to the calculation of spectral properties in realistic electron–phonon-coupled systems in a computationally inexpensive manner with encouraging accuracy.

Atomic and molecular spectra↗
DOE OSTI2019

Mini volume collapse as evidence for a three-body magnetic polaron in S m 1 - x E u x S

Samarium sulfide (SmS) is a nonmagnetic narrow-gap (0.06 eV) semiconductor that undergoes a transition to a metallic intermediate valence state at 6.5 kbar. Europium sulfide (EuS) is a ferromagnetic semiconductor with a Curie temperature of 16 K and a gap of 1.6 eV. Here we present a study of the lattice constant, magnetic susceptibility, and resistivity of the substitution series Sm 1-x Eu x S for 0 < x < 1. We observe a smooth interpolation of magnetic and transport behavior across the series, consistent with a virtual crystal scenario and Vegard’s law. Surprisingly, however, the lattice constant deviates below Vegard’s law in a manner that suggests parametric control of the Sm-Sm distance by the Eu moment in the manner of a magnetic polaron.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Electronic structure and small-hole polarons in YTiO 3

As a prototypical Mott insulator with ferromagnetic ordering, YTiO 3 (YTO) is of great interest in the study of strong electron correlation effects and orbital ordering. Here we report the first molecular beam epitaxy (MBE) growth of YTO films, combined with theoretical and experimental characterizations of the electronic structure and charge transport properties. The obstacles of YTO MBE growth are discussed and potential routes to overcome them are proposed. DC transport and Seebeck measurements on thin films and bulk single crystals identify p-type Arrhenius transport behavior with an activation energy of ~0.17 eV in thin films, consistent with the energy barrier for small hole polaron migration from hybrid density functional theory calculations. Hard x-ray photoelectron spectroscopy measurements show the lower Hubbard band at 1.1 eV below the Fermi level, whereas a Mott-Hubbard band gap of ~1.5 eV is determined from photoluminescence measurements. These findings provide critical insight into the electronic band structure of YTO and related materials.

36 MATERIALS SCIENCE↗
DOE OSTI2013

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

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

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗