Search results for "polaron"
showing 10 items of 79 documents
Semi-Empirical Calculations of Hole Polarons in MgO and KNbO3 Crystals
1998
The semi-empirical quantum chemical INDO method has been used for cluster and large unit cell calculations of hole polarons bound to a cation vacancy in highly ionic MgO and partly covalent perovskite KNbO 3 . In both cases a hole is well localized on an oxygen atom displaced towards the vacancy. The calculated optical and thermal ionization energies for V - and V 0 centers are in excellent agreement with experimental data for MgO. In KNbO 3 we predict the existence of one-site and two-site (molecular) polarons with close absorption energies (1 e V). The relevant experimental data are discussed.
On nature of the transient IR-absorption STE-like bands at 0.15–0.36eV in alkali halides
2001
New evidence is given that two classes (A and B) of the transient IR-absorption bands: (A) with max. at 0.15-0.36 eV (in NaCl : I, NaBr, NaI, KCl : I, KBr : I, RbCl : I, RbBr : I), due to on-centre self-trapped exciton and (B) with max. at 0.27-0.36 eV (in NaCI, KCl, KBr, RbCl), due to shallow trapped electrons or bound polarons, are caused by the same defect-shallow trapped electron (e-) at the substitutional (cation: c-site) alkali impurity cation (M + ): [M - ] 0 c e - . The A- and B-class IR bands have the same location, similar shape, half-width (exactly coincide for KCl : I and KCl at 80 or 10 K with the same vibration structure). It is established that the same Mollwo-Ivey plot curve…
The role of Fe and Cu dopants in electron–hole trapping and relaxation process in congruent LiNbO3
2003
Abstract The transient optical absorption and kinetics of absorption decay is studied in undoped, Fe doped, and Cu doped LiNbO 3 crystals irradiated by pulsed electron beam. The 1.6 eV band of electron polaron trapped at antisite niobium was observed in all crystal samples. The nature of centers responsible for transient absorption is discussed. Electron polarons are shown to be less stable in LiNbO 3 :Fe compared with LiNbO 3 :Cu and undoped LiNbO 3 . It is suggested that a major part of electrons and holes created by irradiation are trapped in the vicinity of dopants.
Quantum chemical modelling of electron polarons and excitons in ABO3perovskites
2000
Quantum chemical calculations using the intermediate neglect of the differential overlap (INDO) method, combined with the large unit cell periodic model argue for an existence of the self-trapped electrons in KNbO3 and KTaO3 perovskite crystals. An electron in the ground state occupies predominantly t2g orbital of a Nb4+ ion. Its orbital degeneracy is lifted by a combination of the breathing and Jahn-Teller modes where four nearest equatorial O atoms are displaced outwards and two oxygens shift inwards along the z axis. Triplet exciton is shown to be in a good approximation of a pair of nearest Jahn-Teller electron and hole polarons (a bipolaron) which is very likely responsible for the `gr…
Frequency and temperature dependence of the electrical conductivity of KTaO3; Li and PbTiO3; La, Cu: Indication of a low temperature polaron mechanism
2008
Abstract Recently, the concept of polarons has again been at the focus of solid-state research, as it can constitute the basis for understanding the high-temperature superconductivity or the colossal magnetoresistance of materials. More than a decade ago there were some indications that polarons play an important role in explaining low temperature maxima in imaginary part of the dielectric constant e ″ ( T ) in ABO3 perovskites. In the present work we report the ac electrical conductivities of KTaO3; Li and PbTiO3; La, Cu and their frequency and temperature dependence. The real part of the complex ac conductivity was found to follow the universal dielectric response σ ′ ∝ ν s . A detailed t…
Quantum Mechanical Modelling of Pure and Defective KNbO3 Perovskites
2000
Ab initio electronic structure calculations using the density-functional theory (DFT) are performed for KNbO3 with and without defects. Ferroelectric distortive transitions involve very small changes in energies and are therefore sensitive to DFT-approximations. This is discussed by comparing results obtained with the local density approximation (LDA) to those where generalized gradient approximations (GGA) are used. The results of ab initio calculations for F-type centers and bound hole polarons are compared to those obtained by a semiempirical method of the Intermediate Neglect of the Differential Overlap (INDO), based on the HartreeFock formalism. Supercells with 40 and 320 atoms were us…
<title>Computer modeling of point defects, polarons, excitons, and surfaces in perovskite ferroelectrics</title>
2003
We review results of our recent large-scale computer simulations of point defects, excitons and polarons in ABO3 perovskite crystals, focusing mostly on KNbO3 and KTaO3 as representative examples. We have calculated the atomic and electronic structure of defects, their optical absorption and defect-induced electron density redistribution. The majority of results are obtained using the quantum chemical method of the intermediate neglect of differential overlap (INDO) based on the Hartree-Frock formalism. The main findings are compared with results of ab initio Density Functional Theory (FP-LMTO) first-principles calculations. The results of the electronic structure calculations for different…
Polaronic relaxation in perovskites
1995
We report a low-temperature loss anomaly in several oxidic perovskites such as ${\mathrm{KTaO}}_{3}$, ${\mathrm{KTaO}}_{3}$:Nb, ${\mathrm{SrTiO}}_{3}$, ${\mathrm{SrTiO}}_{3}$:Ca, ${\mathrm{PbTiO}}_{3}$:La, Cu, and ${\mathrm{BaTiO}}_{3}$:La. We show that this anomaly arises from a low-frequency dielectric relaxation. The activation energy and the relaxation time of this process are nearly the same for all the investigated perovskites disregarding their composition, texture, and ferroelectric properties. We thus ascribe the loss anomaly to the localization of polarons on residual defects. Although the dielectric losses in ${\mathrm{SrTiO}}_{3}$ and ${\mathrm{SrTiO}}_{3}$:Ca are qualitatively …
Calculations of radiation-induced point defects, polarons and excitons in ferroelectric perovskites
2002
Abstract We review results of our recent large-scale computer simulations of radiation-induced point defects, excitons and polarons in ABO3 perovskite crystals, focusing mostly on KNbO3 and KTaO3 as representative examples. We have calculated the atomic and electronic structure of defects, their optical absorption, defect-induced electron density redistribution, and activation energies for defect migration. The majority of our results were obtained using the quantum-chemical method of the intermediate neglect of differential overlap (INDO) based on the Hartree–Fock formalism, as well as the shell model (SM). The main findings are compared with those obtained by means of ab initio density fu…
Large scale computer modelling of point defects in ABO 3 perovskites
2005
We present results for basic intrinsic defects: F-type electron centers, free and bound electron and hole polarons in ABO3 perovskites. Both one-site (atomic) and two-site (molecular) hole polarons are expected to coexist, characterized by close absorption energies. Shell Model (SM) and intermediate neglect of differential overlap (INDO) calculations of the F center diffusion indicate that the relevant activation energy is quite low, ca. 0.8 eV. Further INDO calculations support the existence of self-trapped electron polarons in PbTiO3, BaTiO3, KNbO3, and KTaO3 crystals. The relevant lattice relaxation energies are typically 0.2 eV, whereas the optical absorption energies are around 0.8 eV.…