arXiv subjects

Vasili Perebeinos

Publications and source records attributed to Vasili Perebeinos.

72 records · Page 4Linked to original sources

arXiv2005

Mobility in semiconducting carbon nanotubes at finite carrier density

Carbon nanotube field-effect transistors operate over a wide range of electron or hole density, controlled by the gate voltage. Here we calculate the mobility in semiconducting nanotubes as a function of carrier density and electric field, for different tube diameters and temperature. The low-field mobility is a non-monotonic function of carrier density, and varies by as much as a factor of 4 at room temperature. At low density, with increasing field the drift velocity reaches a maximum and then exhibits negative differential mobility, due to the non-parabolicity of the bandstructure. At a critical density $ρ_c\sim$ 0.35-0.5 electrons/nm, the drift velocity saturates at around one third of the Fermi velocity. Above $ρ_c$, the velocity increases with field strength with no apparent saturation.

cond-mat.mtrl-sci↗

arXiv2005

Radiative Lifetime of Excitons in Carbon Nanotubes

We calculate the radiative lifetime and energy bandstructure of excitons in semiconducting carbon nanotubes, within a tight-binding approach. In the limit of rapid interband thermalization, the radiative decay rate is maximized at intermediate temperatures, decreasing at low temperature because the lowest-energy excitons are optically forbidden. The intrinsic phonons cannot scatter excitons between optically active and forbidden bands, so sample-dependent extrinsic effects that break the symmetries can play a central role. We calculate the diameter-dependent energy splittings between singlet and triplet excitons of different symmetries, and the resulting dependence of radiative lifetime on temperature and tube diameter.

cond-mat.mtrl-sci↗

arXiv2004

Exciton-phonon effects in carbon nanotube optical absorption

We find that the optical properties of carbon nanotubes reflect remarkably strong effects of exciton-phonon coupling. Tight-binding calculations show that a significant fraction of the spectral weight of the absorption peak is transferred to a distinct exciton+phonon sideband, which is peaked at around 200 meV above the main absorption peak. This sideband provides a distinctive signature of the excitonic character of the optical transition. The exciton-phonon coupling is reflected in a dynamical structural distortion, which contributes a binding energy of up to 100 meV. The distortion is surprisingly long-ranged, and is strongly dependent on chirality.

cond-mat.mtrl-sci↗

arXiv2004

Electron-phonon effects and transport in carbon nanotubes

We calculate the electron-phonon scattering and binding in semiconducting carbon nanotubes, within a tight binding model. The mobility is derived using a multi-band Boltzmann treatment. At high fields, the dominant scattering is inter-band scattering by LO phonons corresponding to the corners K of the graphene Brillouin zone. The drift velocity saturates at approximately half the graphene Fermi velocity. The calculated mobility as a function of temperature, electric field, and nanotube chirality are well reproduced by a simple interpolation formula. Polaronic binding give a band-gap renormalization of ~70 meV, an order of magnitude larger than expected. Coherence lengths can be quite long but are strongly energy dependent.

cond-mat.mtrl-sci↗

arXiv2004

Electronic structure of S-C6H5 self-assembled monolayers on Cu(111) and Au(111) substrates

We use first principles density functional theory to calculate the electronic structure of the phenylthiolate (S-C$_6$H$_5$) self-assembled monolayer (SAM) on Cu(111) and Au(111) substrates. We find significant lateral dispersion of the SAM molecular states and discuss its implications for transport properties of the molecular wire array. We calculate the two photon photoemission spectra and the work function of the SAM on Cu(111) and compare them with the available experimental data. Our results are used to discuss assignments of the observed spectral data and yield predictions for new electronic states due to the monolayer not yet accessed experimentally.

cond-mat.mtrl-sci↗

arXiv2004

Scaling of excitons in carbon nanotubes

Light emission from carbon nanotubes is expected to be dominated by excitonic recombination. Here we calculate the properties of excitons in nanotubes embedded in a dielectric, for a wide range of tube radii and dielectric environments. We find that simple scaling relationships give a good description of the binding energy, exciton size, and oscillator strength.

cond-mat.mtrl-sci↗

arXiv2003

Investigation of the Jahn-Teller Transition in TiF3 using Density Functional Theory

We use first principles density functional theory to calculate electronic and magnetic properties of TiF3 using the full potential linearized augmented plane wave method. The LDA approximation predicts a fully saturated ferromagnetic metal and finds degenerate energy minima for high and low symmetry structures. The experimentally observed Jahn-Teller phase transition at Tc=370K can not be driven by the electron-phonon interaction alone, which is usually described accurately by LDA. Electron correlations beyond LDA are essential to lift the degeneracy of the singly occupied Ti t2g orbital. Although the on-site Coulomb correlations are important, the direction of the t2g-level splitting is determined by the dipole-dipole interactions. The LDA+U functional predicts an aniferromagnetic insulator with an orbitally ordered ground state. The input parameters U=8.1 eV and J=0.9 eV for the Ti 3d orbital were found by varying the total charge on the TiF$_6^{2-}$ ion using the molecular NRLMOL code. We estimate the Heisenberg exchange constant for spin-1/2 on a cubic lattice to be approximately 24 K. The symmetry lowering energy in LDA+U is about 900 K per TiF3 formula unit.

cond-mat.mtrl-sci↗

arXiv2003

Density Functional Study of Cubic to Rhombohedral Transition in $α$-AlF$_3$

Under heating, $α$-AlF$_3$ undergoes a structural phase transition from rhombohedral to cubic at temperature $T$ around 730 K. The density functional method is used to examine the $T$=0 energy surface in the structural parameter space, and finds the minimum in good agreement with the observed rhombohedral structure. The energy surface and electronic wave-functions at the minimum are then used to calculate properties including density of states, $Γ$-point phonon modes, and the dielectric function. The dipole formed at each fluorine ion in the low temperature phase is also calculated, and is used in a classical electrostatic picture to examine possible antiferroelectric aspects of this phase transition.

cond-mat.mtrl-sci↗

arXiv2003

Jahn-Teller instability in C6H6+ and C6H6- revisited

The benzene cation (C6H6+) has a doublet (e_{1g}) ground state in hexagonal ring (D_{6h}) geometry. Therefore a Jahn-Teller (JT) distortion will lower the energy. The present theoretical study yields a model Huckel-type Hamiltonian that includes the JT coupling of the e_{1g} electronic ground state with the two e_{2g} vibrational modes: in-plane ring-bending and C-C bond-stretching. We obtain the JT couplings from density functional theory (DFT), which gives a JT energy lowering of 970 cm^{-1} in agreement with previous quantum chemistry calculations. We find a non-adiabatic solution for vibrational spectra and predict frequencies shifts of both the benzene cation and anion, and give a reinterpretation of the available experimental data.

cond-mat↗

arXiv2002

"Madelung model" prediction for dependence of lattice parameter on nanocrystal size

The competition between the long range Coulomb attractive and the short range repulsive interaction in ionic nanocrystals creates an effective negative pressure, which causes the lattice parameter a to increase with decreasing nanoparticle size d. A simple ``Madelung model'' is used to predict the dependence of the lattice parameter for CeO2 and BaTiO3 on d, delta a/a = alpha/d, for alpha = 0.22 A and 0.18 A respectively. The model predictions are compared with experimental results.

cond-mat.mtrl-sci↗

arXiv2001

Polaronic Signatures in Mid-Infrared Spectra: Prediction for LaMnO3 and CaMnO3

Hole-doped LaMnO3 and electron-doped CaMnO3 form self-trapped electronic states. The spectra of these states have been calculated using a two orbital (Mn eg Jahn-Teller) model, from which the non-adiabatic optical conductivity spectra are obtained. In both cases the optical spectrum contains weight in the gap region, whose observation will indicate the self-trapped nature of the carrier states. The predicted spectra are proportional to the concentration of the doped carriers in the dilute regime, with coefficients calculated with no further model parameters.

cond-mat.str-el↗

arXiv2001

Multi-phonon Resonant Raman Scattering Predicted in LaMnO3 from the Franck-Condon Process via Self-Trapped Excitons

Resonant behavior of the Raman process is predicted when the laser frequency is close to the orbital excitation energy of LaMnO3 at 2 eV. The incident photon creates a vibrationally excited self-trapped ``orbiton'' state from the orbitally-ordered Jahn-Teller (JT) ground state. Trapping occurs by local oxygen rearrangement. Then the Franck-Condon mechanism activates multiphonon Raman scattering. The amplitude of the $n$-phonon process is first order in the electron-phonon coupling $g$. The resonance occurs {\it via} a dipole forbidden $d$ to $d$ transition. We previously suggested that this transition (also seen in optical reflectivity) becomes allowed because of asymmetric oxygen fluctuations. Here we calculate the magnitude of the corresponding matrix element using local spin-density functional theory. This calculation agrees to better than a factor of two with our previous value extracted from experiment. This allows us to calculate the absolute value of the Raman tensor for multiphonon scattering. Observation of this effect would be a direct confirmation of the importance of the JT electron-phonon term and the presence of self-trapped orbital excitons, or ``orbitons''.

cond-mat.str-el↗

arXiv2000

Exact, numerical, and mean field behavior of a dimerizing lattice in one dimension

The thermodynamics and dynamics of a one dimensional dimer-forming anharmonic model is studied in the classical limit. This model mimics the behavior of materials with a Peierls instability. Specific heat, correlation length, and order parameter are calculated three ways: (a) by mean field approximation, (b) by numerical molecular dynamics simulation, and (c) by an exact transfer matrix method. The single-particle spectrum (velocity-velocity correlation function) is found numerically and in mean field theory.

cond-mat.stat-mech↗

arXiv2000

Franck-Condon-Broadened Angle-Resolved Photoemission Spectra Predicted in LaMnO3

The sudden photohole of least energy created in the photoemission process is a vibrationally excited state of a small polaron. Therefore the photoemission spectrum in LaMnO3 is predicted to have multiple Franck-Condon vibrational sidebands. This generates an intrinsic line broadening approximately 0.5 eV. The photoemission spectral function has two peaks whose central energies disperse with band width approximately 1.2 eV. Signatures of these phenomena are predicted to appear in angle-resolved photoemission spectra.

cond-mat.str-el↗

arXiv2000

First-principles calculations of the self-trapped exciton in crystalline NaCl

The atomic and electronic structure of the lowest triplet state of the off-center (C2v symmetry) self-trapped exciton (STE) in crystalline NaCl is calculated using the local-spin-density (LSDA) approximation. In addition, the Franck-Condon broadening of the luminescence peak and the a1g -> b3u absorption peak are calculated and compared to experiment. LSDA accurately predicts transition energies if the initial and final states are both localized or delocalized, but 1 eV discrepancies with experiment occur if one state is localized and the other is delocalized.

cond-mat.str-el↗

arXiv1999

Self-trapped Exciton and Franck-Condon Spectra Predicted in LaMnO$_3$

Because the ground state has cooperative Jahn-Teller order, electronic excitations in LaMnO$_3$ are predicted to self-trap by local rearrangement of the lattice. The optical spectrum should show a Franck-Condon series, that is, a Gaussian envelope of vibrational sidebands. Existing data are reinterpreted in this way. The Raman spectrum is predicted to have strong multiphonon features.

cond-mat.str-el↗

arXiv1999

Toward a Theory of Orbiton Dispersion in LaMnO_3

At 750K, LaMnO_3 has a cooperative Jahn-Teller (JT) distortion, with Mn atoms in distorted oxygen octahedra. This lifts the degeneracy of the singly-occupied $e_g$ orbitals of the Mn$^{3+}$ ions, which then become orbitally ordered. We use a minimal model to describe the ordered phase at T=0. The on-site Coulomb repulsion $U$ is set to infinity. There are two electronic orbitals and three oxygen vibrational coordinates per unit cell. In addition to spin excitations and phonons, the model has electronic excitations consisting of mis-orienting orbitals on Mn ions. Neglecting coupling to the oxygen displacements, the gap to such excitations is $2Δ=16g^2/K$ where $g$ is the electron-phonon coupling and $K$ is the oxygen spring constant. When static oxygen displacements are coupled, this excitation becomes a self-trapped exciton with energy $Δ$, half the JT gap. Adding dynamic oxygen displacements in one-phonon approximation introduces dispersion to both the (previously Einstein-like) phonons and the orbital excitons (``orbitons''). One of the phonon branches has zero frequency at $\vec{k}=(0,0,π)$. This is the Goldstone mode of the JT broken symmetry.

cond-mat.str-el↗

arXiv1999

The Anti-Jahn-Teller Polaron in LaMnO$_3$

Distortions of the oxygen sublattice couple to $e_g$ orbitals of Mn$^{3+}$ and drive a cooperative Jahn-Teller (orbital ordering) transition in LaMnO$_3$. A simple model for this transition is studied. Without further adjustment, the model predicts the shape and stability of small (anti-Jahn-Teller) polarons which form when holes are doped into the material. This leads to a new description of the lightly doped insulator, the anti-ferromagnetic to ferromagnetic transition, and the metal-insulator transition.

cond-mat.str-el↗