化学物理
A kernel-based method (kernelized minimal distributed charge model - kMDCM) to represent the molecular electrostatic potential (ESP) in terms of off-center point charges whose positions adapts to the molecular geometry. Using Gaussian…
Carbon quantum dots have become attractive in various applications, such as drug delivery, biological sensing, photocatalysis, and solar cells. Among these, pH sensing via luminescence lifetime measurements of surface-functionalised carbon…
This paper introduces the combination of an advanced double-layer model with electrochemical kinetics to explain electrolyte effects on the alkaline hydrogen evolution reaction. It is known from experimental studies that the alkaline…
In this work, rate coefficients of four prototypical insertion reactions, X + H2 -- H + XH (X=C(1D), N(2D), O(1D), S(1D)) and associated isotope reactions are calculated based on ring polymer molecular dynamics (RPMD) with Cayley propagator…
Solvent interactions, particularly hydration, are vital in chemical and biochemical systems. Model systems unveil microscopic details of such interactions. We uncover a specific hydrogen-bonding motif of the biomolecular building block…
Machine Learning (ML)-based force fields are attracting ever-increasing interest due to their capacity to span spatiotemporal scales of classical interatomic potentials at quantum-level accuracy. They can be trained based on high-fidelity…
We have presented the theory, implementation, and benchmark results for the one-electronic variant of spin-free exact two-component (SFX2C1e) linear response coupled cluster (LRCCSD) theory for static and dynamic polarizabilities of atoms…
Burning fossil fuels emits a significant amount of CO2, causing climate change concerns. CO2 Capture and Storage (CCS) aims to reduce emissions, with fullerenes showing promise as CO2 adsorbents. Recent research focuses on modifying…
Recently we investigated from first principles screening properties in systems where small molecules, characterized by a finite electronic dipole moment, are encapsulated into different nanocages. The most relevant result was the…
The general theoretical description of spin self-diffusion under nonlinear gradient is proposed, which extends the effective phase diffusion method for linear gradient field. Based on the phase diffusion, the proposed method reveals the…
This work introduces a comprehensive approach utilizing data-driven methods to elucidate the deposition process regimes in Chemical Vapor Deposition (CVD) reactors and the interplay of physical mechanism that dominate in each one of them.…
We introduce a machine learning (ML) supervised model function that is inspired by the variational principle of physics. This ML hypothesis evolutionary method, termed ML-Omega, allows us to go from data to differential equation(s)…
The adsorption and desorption of reactants and products from a solid surface is essential for achieving sustained surface chemical reactions. At a liquid-solid interface, these processes can involve the collective reorganization of…
Various condensed phases of water, spanning from the liquid state to multiple ice phases, have been systematically investigated under extreme conditions of pressure and temperature to delineate their stability boundaries. This study focuses…
The surface of Saturn's moon Titan is coated with small molecule organic solids termed cryominerals. Cryominerals play an analogous role to minerals on Earth in Titan's surface geology and geochemistry. To develop a predictive understanding…
A recent experimental study reports on measuring the temporal duration and the spatial extent of failed attempts to cross an activation barrier (i.e., "loops") for a folding transition in a single molecule and for a Brownian particle…
We introduce a novel algorithm that leverages stochastic sampling techniques to compute the perturbative triples correction in the coupled-cluster (CC) framework. By combining elements of randomness and determinism, our algorithm achieves a…
Attochemistry aims to exploit the properties of coherent electronic wavepackets excited via attosecond pulses, to control the formation of photoproducts. Such molecular processes can in principle be simulated with various nonadiabatic…
Non-adiabatic dynamics simulations have become a standard approach to explore photochemical reactions. Such simulations require underlying potential energy surfaces and couplings between them, calculated at a chosen level of theory, yet…
Photoionized and electronically excited ethylene \ce{C2H4+} can undergo \ce{H}-loss, \ce{H2}-loss, and ethylene-ethylidene isomerization, where the latter entails a hydrogen migration. Recent pioneering experiments with few-femtosecond…