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We study the effect of quantum vibronic coupling on the electronic properties of carbon allotropes, including molecules and solids, by combining path integral first principles molecular dynamics (FPMD) with a colored noise thermostat. In…

Materials Science · Physics 2021-08-04 Arpan Kundu , Marco Govoni , Han Yang , Michele Ceriotti , Francois Gygi , Giulia Galli

The renormalization of the band structure at zero temperature due to electron-phonon coupling is investigated in diamond, BN, LiF and MgO crystals. We implement a dynamical scheme to compute the frequency-dependent self-energy and the…

Diamond is studied by path integral molecular dynamics simulations of the atomic nuclei in combination with a tight-binding Hamiltonian to describe its electronic structure and total energy. This approach allows us to quantify the influence…

Materials Science · Physics 2009-11-11 Rafael Ramirez , Carlos P. Herrero , Eduardo R. Hernandez

We investigate the impact of quantum vibronic coupling on the electronic properties of solid-state spin defects using stochastic methods and first principles molecular dynamics with a quantum thermostat. Focusing on the negatively charged…

Computational Physics · Physics 2024-01-19 Arpan Kundu , Giulia Galli

We present an accurate computational study of the electronic structure and lattice dynamics of solid molecular hydrogen at high pressure. The band-gap energies of the $C2/c$, $Pc$, and $P6_3/m$ structures at pressures of 250, 300, and 350…

Materials Science · Physics 2017-10-27 Sam Azadi , Ranber Singh , T. D. Kühne

We develop a first-principles approach for the treatment of vibronic interactions in solids that overcomes the main limitations of state-of-the-art electron-phonon coupling formalisms. In particular, anharmonic effects in the nuclear…

Materials Science · Physics 2020-07-29 Marios Zacharias , Matthias Scheffler , Christian Carbogno

Diamondoids are a unique form of carbon nanostructure best described as hydrogen-terminated diamond molecules. Their diamond-cage structures and tetrahedral sp3 hybrid bonding create new possibilities for tuning electronic band gaps,…

Electronic and optical properties of materials are affected by atomic motion through the electron-phonon interaction: not only band gaps change with temperature, but even at absolute zero temperature, zero-point motion causes band-gap…

The frozen-phonon method, used to calculate electron-phonon coupling effects, requires calculations of the investigated structure using atomic coordinates displaced according to a certain phonon eigenmode. The process of "freezing-in" the…

Chemical Physics · Physics 2019-04-12 Pablo García-Risueño , Peng Han , Gabriel Bester

Effects of nuclear dynamics on the energetics of polythiophene relevant for the performance of organic solar cells are studied for the first time. Nuclear motions change the expectation values of frontier orbital energies and the band gap…

Chemical Physics · Physics 2016-02-05 Sergei Manzhos

Here we present theoretical studies of the effect of vibronic coupling on nonlinear transport characteristics (current-voltage and conductance-voltage) in molecular electronic devices. Considered device is composed of molecular quantum dot…

Mesoscale and Nanoscale Physics · Physics 2009-11-11 Kamil Walczak

Anharmonic atomic motions can strongly influence the optoelectronic properties of materials but how these effects are connected to the underlying phonon band structure is not understood well. We investigate how the electronic band gap is…

Materials Science · Physics 2024-06-11 Xiangzhou Zhu , David A. Egger

We present density-functional theory (DFT) and quantum Monte Carlo (QMC) calculations designed to resolve experimental and theoretical controversies over the optical properties of H-terminated C nanoparticles (diamondoids). The QMC results…

Materials Science · Physics 2008-01-03 N. D. Drummond , A. J. Williamson , R. J. Needs , G. Galli

Lattice vibrations within crystalline solids, or phonons, provide information on a variety of important material characteristics, from thermal qualities to optical properties and phase transition behaviour. When the material contains light…

Computational Physics · Physics 2025-06-27 Taylor Baird , Rodolphe Vuilleumier , Sara Bonella

Accurate electronic bandstructures of solids are indispensable for a wide variety of applications and should provide a sound prediction of phonon-induced band gap renormalization at finite temperatures. We employ our previously introduced…

Computational Physics · Physics 2024-03-22 Tammo van der Heide , Ben Hourahine , Bálint Aradi , Thomas Frauenheim , Thomas A. Niehaus

We present a vibrational dynamical mean-field theory (VDMFT) of the dynamics of atoms in solids with anharmonic interactions. Like other flavors of DMFT, VDMFT maps the dynamics of a periodic anharmonic lattice of atoms onto those of a…

Materials Science · Physics 2022-08-10 Petra Shih , Timothy C. Berkelbach

We introduce a general approach for the simulation of quantum vibrational states of (symmetric and asymmetric) double-well potentials in molecules and materials for thermodynamic and spectroscopic applications. The method involves solving…

Organic molecular crystals are expected to feature appreciable electron-phonon interactions that influence their electronic properties at zero and finite temperature. In this work, we report first-principles calculations and an analysis of…

We present a method to efficiently combine the computation of electron-electron and electron-phonon self-energies, which enables the evaluation of electron-phonon coupling at the $G_0W_0$ level of theory for systems with hundreds of atoms.…

Materials Science · Physics 2021-12-14 Han Yang , Marco Govoni , Arpan Kundu , Giulia Galli

Phonon properties of realistic materials are routinely calculated within the Density Functional Perturbation Theory\,(DFPT). This is a semi--classical approach where the atoms are assumed to oscillate along classical trajectories immersed…

Materials Science · Physics 2024-07-24 Andrea Marini
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