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The application of molecular dynamics (MD) simulations to the interpretation of Raman scattering spectra is hindered by inability of atomistic simulations to account for the dynamic evolution of electronic polarizability, requiring the use…

Materials Science · Physics 2023-04-18 Atanu Paul , Anthony Ruffino , Stefan Masiuk , Jonathan Spanier , Ilya Grinberg

Raman spectroscopy is an important tool for studies of molecules, liquids and solids. While Raman spectra can be obtained theoretically from molecular dynamics (MD) simulations, this requires the calculation of the electronic polarizability…

Materials Science · Physics 2025-01-22 Atanu Paul , Nagaprasad Reddy Samala , Ilya Grinberg

Calculation of Raman scattering from molecular dynamics (MD) simulations requires accurate modeling of the evolution of the electronic polarizability of the system along its MD trajectory. For large systems, this necessitates the use of…

Materials Science · Physics 2024-06-12 Atanu Paul , Maya Rubenstein , Anthony Ruffino , Stefan Masiuk , Jonathan Spanier , Ilya Grinberg

We present a new formulation of ab initio molecular dynamics which exploits the efficiency of plane waves in adaptive curvilinear coordinates, and thus provides an accurate treatment of first-row elements. The method is used to perform a…

mtrl-th · Physics 2009-10-28 Francois Gygi

We present a computational method to accurately calculate Raman spectra from first principles with an at least one order of magnitude higher efficiency. This scheme thus allows to routinely calculate finite-temperature Raman spectra…

Chemical Physics · Physics 2015-04-15 Pouya Partovi-Azar , Thomas D. Kühne

A new approach to simulating warm and hot dense matter that combines density functional theory based calculations of the electronic structure to classical molecular dynamics simulations with pair interaction potentials is presented. The new…

Plasma Physics · Physics 2015-06-22 C. E. Starrett , J. Daligault , D. Saumon

Accounting for electrons and nuclei simultaneously is a powerful capability of ab initio molecular dynamics (AIMD). However, AIMD is often unable to accurately reproduce properties of systems such as water due to inaccuracies in the…

Chemical Physics · Physics 2017-01-25 Andrew D. White , Chris Knight , Glen M. Hocky , Gregory A. Voth

In this work, we develop a framework for atomistic modeling of electronic polarizability to predict the Raman spectra of hydrogen-bonded clusters and liquids from molecular dynamics (MD) simulations. The total polarizability of the system…

Chemical Physics · Physics 2025-03-25 Atanu Paul , Ilya Grinberg

An accurate treatment of the structures and dynamics that lead to enhanced chemical reactivity in enzymes requires explicit treatment of both electronic and nuclear quantum effects. The former can be captured in ab initio molecular dynamics…

Chemical Physics · Physics 2022-08-26 Lu Wang , Christine M. Isborn , Thomas E. Markland

This paper reviews Irradiation Driven Molecular Dynamics (IDMD) - a novel computational methodology for atomistic simulations of the irradiation driven transformations of complex molecular systems implemented in the MBN Explorer software…

Chemical Physics · Physics 2023-09-06 Alexey V. Verkhovtsev , Ilia A. Solov'yov , Andrey V. Solov'yov

Based on a linearization approximation coupled with path integral formalism, we propose a method derived from the propagation of quasi-classical trajectories to simulate resonance Raman spectra. This method is based on a ground state…

Chemical Physics · Physics 2023-07-26 Hugo Bessone , Rodolphe Vuilleumier , Riccardo Spezia

Raman spectroscopy is an important tool in the study of vibrational properties and composition of molecules, peptides and even proteins. Raman spectra can be simulated based on the change of the electronic polarizability with vibrations,…

Computational Physics · Physics 2024-04-30 Ethan Berger , Juha Niemelä , Outi Lampela , André H. Juffer , Hannu-Pekka Komsa

We present a new method to compute resonance Raman spectra based on ab initio level calculations using the frequency-dependent Placzek approximation. We illustrate the efficiency of our hybrid quantum-classical method by calculating the…

Other Condensed Matter · Physics 2019-04-09 Gergő Kukucska , Viktor Zólyomi , János Koltai

We describe a new approach based on semiclassical molecular dynamics that allows to simulate infrared absorption or emission spectra of molecular systems with inclusion of anharmonic intensities. This is achieved from semiclassical power…

Chemical Physics · Physics 2018-11-12 Marco Micciarelli , Riccardo Conte , Jaime Suarez , Michele Ceotto

Raman spectroscopy is a powerful and nondestructive method that is widely used to study the vibrational properties of solids or molecules. Simulations of finite-temperature Raman spectra rely on obtaining polarizabilities along molecular…

Mesoscale and Nanoscale Physics · Physics 2023-10-23 Ethan Berger , Hannu-Pekka Komsa

For 35 years, {\it ab initio} molecular dynamics (AIMD) has been the method of choice for modeling complex atomistic phenomena from first principles. However, most AIMD applications are limited by computational cost to systems with…

Computational Physics · Physics 2020-09-15 Weile Jia , Han Wang , Mohan Chen , Denghui Lu , Lin Lin , Roberto Car , Weinan E , Linfeng Zhang

Line-by-line calculations are becoming the standard procedure for carrying spectral simulations. However, it is important to insure the accuracy of such spectral simulations through the choice of adapted models for the simulation of key…

Optics · Physics 2007-05-23 M. Lino da Silva

We present and evaluate an efficient method for simulating Raman spectra from molecular dynamics (MD) calculations {\it without} defining normal modes. We apply the method to high pressure hydrogen in the high-temperature "Phase IV": a…

Materials Science · Physics 2014-08-19 G. J. Ackland , I. B. Magdau

A new "on the fly" method to perform Born-Oppenheimer ab initio molecular dynamics (AIMD) is presented. Inspired by Ehrenfest dynamics in time-dependent density functional theory, the electronic orbitals are evolved by a Schroedinger-like…

We present it ab-initio calculations of the non-resonant Raman spectra of zigzag and armchair BN nanotubes. In comparison, we implement a generalized bond-polarizability model where the parameters are extracted from first-principles…

Materials Science · Physics 2013-08-07 Ludger Wirtz , Michele Lazzeri , Francesco Mauri , Angel Rubio
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