化学物理
Thiolate containing mercury(II) complexes of the general formula [Hg(SR)$_n$]$^{2-n}$ have been of great interest since the toxicity of mercury was recognized. $^{199}$Hg nuclear magnetic resonance spectroscopy (NMR) is a powerful tool for…
Solar redox flow batteries (SRFB) have received much attention as an alternative integrated technology for simultaneous conversion and storage of solar energy. Yet, the photocatalytic efficiency of semiconductor-based single photoelectrode,…
The study of cycloaddition mechanisms is central to the fabrication of extended sp2 carbon nanostructures. Reaction modeling in this context has focused mostly on putative, energetically preferred, exothermic products with limited…
Quantum Monte Carlo (QMC) is a powerful method to calculate accurate energies and forces for molecular systems. In this work, we demonstrate how we can obtain accurate QMC forces for the fluxional ethanol molecule at room temperature by…
To all appearances, electron impact mass spectrometer (EI-MS) is considered a "chirally blind" instrument. Yet, numerous non-identical R (right) and S (left) configurations of prochiral alcohols' mass spectra alcohols have appeared in the…
Characterizing the photolysis processes undergone by transient volatile organic compounds in the troposphere requires the knowledge of their photoabsorption cross-section - quantities often challenging to determine experimentally,…
Local electronic-structure methods in quantum chemistry operate on the ability to compress electron correlations more efficiently in a basis of spatially localized molecular orbitals than in a parent set of canonical orbitals. However, many…
This work combines state-of-the-art machine learning techniques with highest-level electronic structure calculations and full-dimensional quantum tunneling calculations to obtain a quantitative characterization of tunneling splittings for…
The exponential scaling of complete active space (CAS) and full configuration interaction (CI) calculations limits the ability of quantum chemists to simulate the electronic structures of strongly correlated systems. Herein, we present…
Strong coupling of organic molecules to the vacuum field of a nanoscale cavity can be used to modify their chemical and physical properties. We extend the Tavis-Cummings model for molecular ensembles and show that the often neglected…
Nanographene-based magnetism at interfaces offers an avenue to designer quantum materials towards novel phases of matter and atomic-scale applications. Key to spintronics applications at the nanoscale is bistable spin-crossover which…
In this study, we investigated numerically the backdraft phenomenon under different gravity conditions and 4 openings using Fire Dynamics Simulator (FDS) code. Four different opening geometries are studied under ten different gravity…
In the self-consistent continuum solvation (SCCS) approach ($\textit{J. Chem. Phys.}$ 136, 064102 (2012)), the analytical expressions of the local solute-solvent interface functions determine the interface function and dielectric function…
The simple ultraviolet absorption spectrum of thiophene is investigated using a combination of a vibronic coupling model Hamiltonian with multi-configuration time-dependent Hartree quantum dynamics simulations. The model includes five…
We present a new methodology to calculate the strong light-matter coupling between photonic modes in microcavities and large molecular aggregates that consist of hundreds of molecular fragments. To this end, we combine our fragment…
Reactions in solution require "contact" between the reagents. We can predict the rate at which reagents come into "contact" (at least in dilute conditions), but if the initial collision does not lead to reaction, what happens then? The…
We show that a phase space electronic Hamiltonian $\hat{H}_{PS}(\mathbf{X},\mathbf{P})$, parameterized by both nuclear position $\mathbf{X}$ and momentum $\mathbf{P}$, can recover not just experimental vibrational circular dichroism (VCD)…
The successful application of machine learning (ML) in catalyst design relies on high-quality and diverse data to ensure effective generalization to novel compositions, thereby aiding in catalyst discovery. However, due to complex…
We revisit the problem of unphysical charge density delocalization/fractionalization induced by the self-interaction error of common approximate Kohn-Sham Density Functional Theory functionals on simulation of small to medium-size proteins…
This study evaluates the precision of widely recognized quantum chemical methodologies, CCSD(T), DLPNO-CCSD(T) and localized ph-AFQMC, for determining the thermochemistry of main group elements. DLPNO-CCSD(T) and localized ph-AFQMC, which…