Observations on the Electronic Character of Anions and Cations near Water Liquid/Vapor Interfaces DOI
Jack Simons

The Journal of Physical Chemistry A, Год журнала: 2024, Номер unknown

Опубликована: Сен. 18, 2024

In recent years, many researchers have become interested in chemical reactions, photon-induced processes, and other events taking place at or near aqueous liquid/vapor ice/vapor interfaces. Such studies relate to a wide variety of atmospheric, oceanographic, environmental issues. Near these interfaces, atomic molecular anions cations display quite different behaviors than when they are fully solvated the bulk medium. When exist an interface, some capture excess electron produce new neutral-molecule electronic states. Some such can use attached assist hydrolyzing one their first-solvent-shell molecules. Anions residing interface less solvent-stabilized bulk, causing binding energies decrease as approach result which ability act reducing agents increases. Many multiply charged even electronically metastable with respect loss interface. Thus, for both anions, it is important develop tools characterizing varying electronic-state nature migrate between solvation liquid-vapor positioning.

Язык: Английский

Current Status of the MB-pol Data-Driven Many-Body Potential for Predictive Simulations of Water Across Different Phases DOI
Etienne Palos, Ethan F. Bull-Vulpe, Xuanyu Zhu

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2024, Номер 20(21), С. 9269 - 9289

Опубликована: Окт. 14, 2024

Developing a molecular-level understanding of the properties water is central to numerous scientific and technological applications. However, accurately modeling through computer simulations has been significant challenge due complex nature hydrogen-bonding network that molecules form under different thermodynamic conditions. This complexity led over five decades research many attempts. The introduction MB-pol data-driven many-body potential energy function marked advancement toward universal molecular model capable predicting structural, thermodynamic, dynamical, spectroscopic across all phases. By integrating physics-based (i.e., machine-learned) components, which correctly capture delicate balance among interactions, achieves chemical accuracy, enabling realistic water, from gas-phase clusters liquid ice. In this review, we present comprehensive overview formalism adopted by MB-pol, highlight main results predictions made with date, discuss prospects for future extensions potentials generic reactive systems.

Язык: Английский

Процитировано

7
Completely Multipolar Model for Many-Body Water–Ion and Ion–Ion Interactions DOI
Joseph P. Heindel, Lukas Kim, Martin Head‐Gordon

и другие.

The Journal of Physical Chemistry Letters, Год журнала: 2025, Номер unknown, С. 975 - 984

Опубликована: Янв. 21, 2025

This work constructs an advanced force field, the Completely Multipolar Model (CMM), to quantitatively reproduce each term of energy decomposition analysis (EDA) for aqueous solvated alkali metal cations and halide anions their ion pairings. We find that all individual EDA terms remain well-approximated in CMM ion–water ion–ion interactions, except polarization, which shows errors due partial covalency interactions near equilibrium. quantify onset dative bonding regime by examining change molecular polarizability Mayer bond indices as a function distance, showing manifests breaking symmetry atomic polarizabilities while strongly damping them at short-range. motivates environment-dependent parameter depends on strength local electric field experienced ions account strong damping, with anisotropy introduced multipoles. The resulting model provides accurate dimer surfaces three-body polarization charge transfer compared EDA, excellent performance various benchmarks including vibrational frequencies cluster geometries.

Язык: Английский

Процитировано

0
MBX V1.2: Accelerating Data-Driven Many-Body Molecular Dynamics Simulations DOI
Shreya Gupta, Ethan F. Bull-Vulpe, Henry Agnew

и другие.

Journal of Chemical Theory and Computation, Год журнала: 2025, Номер unknown

Опубликована: Фев. 14, 2025

The MBX software provides an advanced platform for molecular dynamics simulations, leveraging state-of-the-art MB-pol and MB-nrg data-driven many-body potential energy functions. Developed over the past decade, these functions integrate physics-based machine-learned terms trained on electronic structure data calculated at "gold standard" coupled-cluster level of theory. Recent advancements in have focused optimizing its performance, resulting release v1.2. While inherently nature ensures high accuracy, it poses computational challenges. v1.2 addresses challenges with significant performance improvements, including enhanced parallelism that fully harnesses power modern multicore CPUs. These enable simulations nanosecond time scales condensed-phase systems, significantly expanding scope high-accuracy, predictive complex systems powered by

Язык: Английский

Процитировано

0
Plasmon enhanced Oxygen Evolution Reaction on Au decorated Ni(OH)2 nanostructures: the role of alkaline cations solvation DOI
Lucas D. Germano, Leonardo D. De Angelis, Ana Paula de Lima Batista

и другие.

Applied Catalysis B Environment and Energy, Год журнала: 2024, Номер 363, С. 124804 - 124804

Опубликована: Ноя. 9, 2024

Язык: Английский

Процитировано

3
Entropy of Liquid Water as Predicted by the Two-Phase Thermodynamic Model and Data-Driven Many-Body Potentials DOI
Ching-Hwa Ho, Francesco Paesani

The Journal of Physical Chemistry B, Год журнала: 2024, Номер 128(28), С. 6885 - 6891

Опубликована: Июль 6, 2024

We investigate the entropy of liquid water at ambient conditions using two-phase thermodynamic (2PT) model, applied to both common pairwise-additive models and MB-pol MB-pol(2023) data-driven many-body potentials. Our simulations demonstrate that 2PT model yields values in semiquantitative agreement with experimental data when MB-pol(2023). Additionally, our analyses indicate predicted by may benefit from error compensation between inherent approximations known limitations these describing interactions. Despite its approximate nature, simplicity makes it a valuable tool for estimating relative changes across various environments, especially combined provide consistently robust representation structural, thermodynamic, dynamical properties water.

Язык: Английский

Процитировано

2
A Novel Ternary Hydrophobic Deep Eutectic Solvent Over a Wide pH Range for Lithium Recovery DOI
Jing‐Lin Chen,

Zhong Tian,

Guisu Yu

и другие.

Journal of Hazardous Materials, Год журнала: 2024, Номер 480, С. 136398 - 136398

Опубликована: Ноя. 7, 2024

Язык: Английский

Процитировано

1
Observations on the Electronic Character of Anions and Cations near Water Liquid/Vapor Interfaces DOI
Jack Simons

The Journal of Physical Chemistry A, Год журнала: 2024, Номер unknown

Опубликована: Сен. 18, 2024

In recent years, many researchers have become interested in chemical reactions, photon-induced processes, and other events taking place at or near aqueous liquid/vapor ice/vapor interfaces. Such studies relate to a wide variety of atmospheric, oceanographic, environmental issues. Near these interfaces, atomic molecular anions cations display quite different behaviors than when they are fully solvated the bulk medium. When exist an interface, some capture excess electron produce new neutral-molecule electronic states. Some such can use attached assist hydrolyzing one their first-solvent-shell molecules. Anions residing interface less solvent-stabilized bulk, causing binding energies decrease as approach result which ability act reducing agents increases. Many multiply charged even electronically metastable with respect loss interface. Thus, for both anions, it is important develop tools characterizing varying electronic-state nature migrate between solvation liquid-vapor positioning.

Язык: Английский

Процитировано

0