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While many vibrational Raman spectroscopy studies of liquid water have investigated the temperature dependence of the high-frequency O-H stretching region, few have analyzed the changes in the Raman spectrum as a function of temperature…

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

Raman spectroscopy is an important characterization tool with diverse applications in many areas of research. We propose a machine learning method for predicting polarizabilities with the goal of providing Raman spectra from molecular…

Materials Science · Physics 2024-02-02 Manuel Grumet , Clara von Scarpatetti , Tomáš Bučko , David A. Egger

We introduce a deep neural network to model in a symmetry preserving way the environmental dependence of the centers of the electronic charge. The model learns from ab-initio density functional theory, wherein the electronic centers are…

Computational Physics · Physics 2020-07-29 Linfeng Zhang , Mohan Chen , Xifan Wu , Han Wang , Weinan E , Roberto Car

In chemical processing and bioprocessing, conventional online sensors are limited to measure only basic process variables like pressure and temperature, pH, dissolved O and CO$_2$ and viable cell density (VCD). The concentration of other…

Quantitative Methods · Quantitative Biology 2020-05-07 Semion Rozov

Vibrational spectroscopy is a key technique to elucidate microscopic structure and dynamics. Without the aid of theoretical approaches, it is however, often difficult to understand such spectra at a microscopic level. Ab initio molecular…

Chemical Physics · Physics 2023-03-14 Philipp Schienbein

Two-dimensional spectroscopic techniques combining terahertz (THz), infrared (IR), and visible pulses offer a wealth of information about coupling among vibrational modes in molecular liquids, thus providing a promising probe of their local…

Chemical Physics · Physics 2023-04-21 Tomislav Begušić , Geoffrey A. Blake

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

Based on deep neural networks (DNNs), deep learning has been successfully applied to many problems, but its mechanism is still not well understood -- especially the reason why over-parametrized DNNs can generalize. A recent statistical…

Disordered Systems and Neural Networks · Physics 2025-06-10 Gang Huang , Lai Shun Chan , Hajime Yoshino , Ge Zhang , Yuliang Jin

We introduce a machine learning prediction workflow to study the impact of defects on the Raman response of 2D materials. By combining the use of machine-learned interatomic potentials, the Raman-active $\Gamma$-weighted density of states…

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

Motivated by the very low diffusivity recently found in ab initio simulations of liquid water, we have studied its dependence with temperature, system size, and duration of the simulations. We use ab initio molecular dynamics (AIMD),…

Soft Condensed Matter · Physics 2009-11-10 M. V. Fernandez-Serra , Emilio Artacho

In this paper we investigate the performance of different machine learning potentials (MLPs) in predicting key thermodynamic properties of water using RPBE+D3. Specifically, we scrutinize kernel-based regression and high-dimensional neural…

Machine learning methods are being explored in many areas of science, with the aim of finding solution to problems that evade traditional scientific approaches due to their complexity. In general, an order parameter capable of identifying…

Soft Condensed Matter · Physics 2017-07-18 Adrián Soto , Deyu Lu , Shinjae Yoo , Mariví Fernández-Serra

We introduce a coarse-grained deep neural network model (CG-DNN) for liquid water that utilizes 50 rotational and translational invariant coordinates, and is trained exclusively against energies of ~30,000 bulk water configurations. Our…

The use of machine learning (ML) algorithms in molecular simulations has become commonplace in recent years. There now exists, for instance, a multitude of ML force field algorithms that have enabled simulations approaching ab initio level…

Chemical Physics · Physics 2025-04-17 Jakub K. Sowa , Peter J. Rossky

We report on an extensive study of the viscosity of liquid water at near-ambient conditions, performed within the Green-Kubo theory of linear response and equilibrium ab initio molecular dynamics (AIMD), based on density-functional theory…

Materials Science · Physics 2022-07-05 Cesare Malosso , Linfeng Zhang , Roberto Car , Stefano Baroni , Davide Tisi

To investigate the possibility of measuring the intermolecular and intramolecular anharmonic coupling of balk water, we calculate third-order two-dimensional (2D) infrared (IR) spectra and fifth-order 2D IR-IR-Raman-Raman spectra expressed…

Soft Condensed Matter · Physics 2023-05-04 Hideaki Takahashi , Yoshitaka Tanimura

The lowest-frequency Raman mode of water, observed through depolarized light scattering or optical Kerr effect techniques, is routinely used to track dynamic changes in water molecules near ions or biomolecules. Yet, the microscopic origin…

Chemical Physics · Physics 2025-11-20 Florian Pabst , Harald Forbert , Dominik Marx

The dielectric permittivity of liquid water is a fundamental property that underlies its distinctive behaviors in numerious physical, biological, and chemical processes. Within a machine learning framework, we present a unified approach to…

Soft Condensed Matter · Physics 2025-08-11 Kehan Cai , Chunyi Zhang , Xifan Wu
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