化学物理
Energy- and resource-efficient electrocatalytic water splitting is of paramount importance to enable sustainable hydrogen production. The best bulk catalyst for the hydrogen evolution reaction (HER), i.e., platinum, is one of the scarcest…
The ability to perform ab initio molecular dynamics simulations using potential energies calculated on quantum computers would allow virtually exact dynamics for chemical and biochemical systems, with substantial impacts on the fields of…
Experimental and computational investigations are carried out to elucidate the influence of ethanol addition on n-heptane auto-ignition in counterflows. An axisymmetric stream of air, temperature gradually increased, is directed onto the…
For electronic systems with multi-reference (MR) character, Kohn-Sham density functional theory (KS-DFT) with the conventional exchange-correlation (xc) energy functionals can lead to incorrect spin densities and related properties. For…
This work studies machine learning for electron density prediction, which is fundamental for understanding chemical systems and density functional theory (DFT) simulations. To this end, we introduce the Gaussian plane-wave neural operator…
Autocatalytic chemical networks play a predominant role in a large number of natural systems such as in metabolic pathways and in ecological networks. Despite recent efforts, the precise impact of thermodynamic constraints on these networks…
The accuracy of phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) can be systematically improved with better trial states. Using multi-Slater determinant trial states, ph-AFQMC has the potential to faithfully treat strongly…
Analytical gradients of potential energy surfaces play a central role in quantum chemistry, allowing for molecular geometry optimizations and molecular dynamics simulations. In strong coupling conditions, potential energy surfaces can…
Ab initio modeling of conical intersection dynamics is crucial for various photochemical, photophysical, and biological processes. However, adiabatic electronic states obtained from electronic structure computations involve random phases,…
We present a detailed investigation of the electronic structure and bonding characteristics of hydrogen-based molecular systems (\ch{H2+}, \ch{H2}, \ch{H2-}) using the Exact Diagonalization Ab Initio (EDABI) approach within the framework of…
The expectation value of the Hamiltonian using a model wave function is widely used to estimate the eigenvalues of electronic Hamiltonians. We explore here a modified formula for models based on long-range interaction. It scales differently…
Upon ionization of an atom or a molecule, another electron (or more) can be simultaneously excited. These concurrently generated states are called "satellites" (or shake-up transitions) as they appear in ionization spectra as higher-energy…
We reexamine $\Delta$CCSD, a state-specific coupled-cluster (CC) with single and double excitations (CCSD) approach that targets excited states through the utilization of non-Aufbau determinants. This methodology is particularly efficient…
Due to the infinite summation of bubble diagrams, the $GW$ approximation of Green's function perturbation theory has proven particularly effective in the weak correlation regime, where this family of Feynman diagrams is important. However,…
Selected configuration interaction (SCI) methods have emerged as state-of-the-art methodologies for achieving high accuracy and generating benchmark reference data for ground and excited states in small molecular systems. However, their…
We investigate the endofullerene system Ne@C$_{70}$, by constructing a three-dimensional Potential Energy Surface (PES) describing the translational motion of the Ne atom. We compare a plethora of electronic structure methods including:…
Ethyl phosphaethyne, C2H5CP, has been characterized spectroscopically in the gas phase for the first time, employing millimeter- and submillimeter-wave spectroscopy in the frequency regime from 75 to 760 GHz. Spectroscopic detection and…
This work is concerned with two-spin-1/2-fermion relativistic quantum mechanics, and it is about the construction of one-particle projectors using an inherently two(many)-particle, `explicitly correlated' basis representation, necessary for…
Despite significant advancements in electrocatalysis for clean hydrogen fuel generation, the transition from concept to commercialization faces challenges due to the instability of electrocatalysts. This study delves into the exploration of…
The software for chemical interaction networks (SCINE) project aims at pushing the frontier of quantum chemical calculations on molecular structures to a new level. While calculations on individual structures as well as on simple relations…