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Aqueous solutions provide a medium for many important reactions in chemical synthesis, industrial processes, environmental chemistry, and biological functions. It is an accepted fact that aqueous solvents can be direct participants to the…

化学物理 · 物理学 2019-08-27 Daniela Polino , Michele Parrinello

The in silico exploration of chemical, physical and biological systems requires accurate and efficient energy functions to follow their nuclear dynamics at a molecular and atomistic level. Recently, machine learning tools gained a lot of…

化学物理 · 物理学 2020-08-26 Silvan Käser , Oliver T. Unke , Markus Meuwly

Simulation techniques based on accurate and efficient representations of potential energy surfaces are urgently needed for the understanding of complex aqueous systems such as solid-liquid interfaces. Here, we present a machine learning…

Molecular dynamics simulations are an important tool for describing the evolution of a chemical system with time. However, these simulations are inherently held back either by the prohibitive cost of accurate electronic structure theory…

化学物理 · 物理学 2018-12-20 Michael Gastegger , Philipp Marquetand

Reactive chemistry of molecular hydrogen at surfaces, notably dissociative sticking and hydrogen evolution, plays a crucial role in energy storage and fuel cells. Theoretical studies can help to decipher underlying mechanisms and reaction…

We present a method to sample reactive pathways via biased molecular dynamics simulations in trajectory space. We show that the use of enhanced sampling techniques enables unconstrained exploration of multiple reaction routes. Time…

计算物理 · 物理学 2020-07-15 Davide Mandelli , Barak Hirshberg , Michele Parrinello

Understanding and prediction of the chemical reactions are fundamental demanding in the study of many complex chemical systems. Reactive molecular dynamics (MD) simulation has been widely used for this purpose as it can offer atomic details…

化学物理 · 物理学 2020-11-12 Jinzhe Zeng , Liqun Cao , Mingyuan Xu , Tong Zhu , John ZH Zhang

Crystal nucleation is relevant across the domains of fundamental and applied sciences. However, in many cases its mechanism remains unclear due to a lack of temporal or spatial resolution. To gain insights to the molecular details of…

软凝聚态物质 · 物理学 2024-04-05 Ziyue Zou , Eric Beyerle , Sun-Ting Tsai , Pratyush Tiwary

Co$_3$O$_4$ is an important catalyst for the oxidation of organic molecules in the liquid phase. Still, understanding the atomistic details of Co$_3$O$_4$-water interfaces under operando conditions remains extremely challenging. While ab…

化学物理 · 物理学 2025-09-03 Amir Omranpour , Jörg Behler

Photo-induced processes are fundamental in nature, but accurate simulations are seriously limited by the cost of the underlying quantum chemical calculations, hampering their application for long time scales. Here we introduce a method…

As the most important solvent, water has been at the center of interest since the advent of computer simulations. While early molecular dynamics and Monte Carlo simulations had to make use of simple model potentials to describe the atomic…

软凝聚态物质 · 物理学 2024-02-01 Amir Omranpour , Pablo Montero De Hijes , Jörg Behler , Christoph Dellago

Using a neural network potential (ANI-1ccx) generated from quantum data on a large data set of molecules and pairs of molecules, isothermal, constant volume simulations demonstrate that the model can be as accurate as ab initio molecular…

化学物理 · 物理学 2021-01-11 Alexander S. Lyons, , Steven W. Rick

The atomic-scale response of inhomogeneous fluids at interfaces and surrounding solute particles plays a critical role in governing chemical, electrochemical and biological processes at such interfaces. Classical molecular dynamics…

A central concern of molecular dynamics simulations are the potential energy surfaces that govern atomic interactions. These hypersurfaces define the potential energy of the system, and have generally been calculated using either predefined…

计算物理 · 物理学 2019-07-05 Emir Kocer , Jeremy K. Mason , Hakan Erturk

Under operating conditions, the dynamics of water and ions confined within protonic aluminosilicate zeolite micropores are responsible for many of their properties, including hydrothermal stability, acidity and catalytic activity. However,…

The reactivity of silicates in an aqueous solution is relevant to various chemistries ranging from silicate minerals in geology, to the C-S-H phase in cement, nanoporous zeolite catalysts, or highly porous precipitated silica. While…

Machine learning techniques including neural networks are popular tools for materials and chemical scientists with applications that may provide viable alternative methods in the analysis of structure and energetics of systems ranging from…

统计力学 · 物理学 2022-03-02 James Andrews , Olga Gkountouna , Estela Blaisten-Barojas

High-fidelity quantum dynamics emulators can be used to predict the time evolution of complex physical systems. Here, we introduce an efficient training framework for constructing machine learning-based emulators. Our approach is based on…

量子物理 · 物理学 2022-03-22 Yu Yao , Chao Cao , Stephan Haas , Mahak Agarwal , Divyam Khanna , Marcin Abram

Oxide-water interfaces govern a wide range of physical and chemical processes fundamental to many fields like catalysis, geochemistry, corrosion, electrochemistry, and sensor technology. Near solid oxide surfaces, water behaves differently…

化学物理 · 物理学 2025-10-31 Jan Elsner , K Nikolas Lausch , Jörg Behler

Hydrodynamic theories effectively describe many-body systems out of equilibrium in terms of a few macroscopic parameters. However, such hydrodynamic parameters are difficult to derive from microscopics. Seldom is this challenge more…

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