化学物理
We develop and numerically analyze an algebraic-geometric framework for spin-adapted coupled-cluster (CC) theory. Since the electronic Hamiltonian is SU(2)-invariant, physically relevant quantum states lie in the spin singlet sector. We…
In this contribution we start by proving and generalizing a conjecture that has been established few decades ago, relating the value of the integral of the detachment/attachment density in two pictures - one accounting for…
Unitary Coupled Cluster (UCC) theory is a promising variational method for electronic structure calculations, especially for strongly correlated systems and quantum computers. However, its practical application is limited by the steep…
Molecular representations are inherently task-dependent, yet most pre-trained molecular encoders are not. Task conditioning promises representations that reorganize based on task descriptions, but existing approaches rely on expensive…
The integration of quantum chemical methods with high-performance computing is indispensable for handling large systems with modest accuracy or even small systems but with high accuracy. Continuing with the unified implementation of…
UGA-SSMRPT2, the spin-free perturbative analogue of Mukerjee's State-Specific Multireference Coupled Cluster Theory (MkMRCC) is known to be successful for size-extensive and intruder-free construction of dissociation curves. This work…
Coulomb explosion imaging (CEI) is a powerful experimental technique that maps a molecule's geometric structure onto the momenta of ionic molecular fragments produced by rapid multiple ionization. Here, we apply CEI induced by pulses from…
Electrochemical cells serve as a building block for producing and storing electrical energy from chemical reactions. The analysis of ion transport in these systems forms the foundation for understanding more complex electrochemical systems…
This work provides a comprehensive theoretical framework for understanding the symmetry properties of High-Resolution NMR spectra. We analyze the conditions under which a spectrum exhibits mirror symmetry (palindromicity). We demonstrate…
We investigate basic hydrogen quantities like the molecular bond length, the molecular dissociation energy and the van-der-Waals interaction in idealized situations in an effort to discern a suitable exchange-correlation functional for the…
The endpoint slippage analysis can be used to quantify the reduction and oxidation side-reactions occurring in rechargeable batteries. Application of this technique often disregards the interference of additional aging modes, such as…
Femtosecond structural dynamics of diiodomethane ($\mathrm{CH_2I_2}$) triggered by ultraviolet (UV) photoabsorption at 290 nm and 330 nm are studied using time-resolved coincident Coulomb explosion imaging driven by a near-infrared probe…
In this study, we present a framework aimed at enhancing molecular property prediction through the integration of local descriptors obtained from large-scale pretrained machine learning potentials into three-dimensional graph neural…
We report on the dynamical measurement of the saturation vapor pressure of $N$-methyl acetamide in the temperature range $-30^\circ$C to $34^\circ$C. This is achieved by monitoring the pressure inside a vacuum chamber in which a precooled…
The simulation of nuclear magnetic resonance (NMR) experiments is a notoriously difficult task, if many spins participate in the dynamics. The recently established dynamic mean-field theory for high-temperature spin systems (spinDMFT)…
Conical intersections (CIs) are seen as the main mediators of nonadiabatic transitions; yet, mixed quantum-classical (MQC) simulations rarely, if ever, sample geometries with exactly degenerate electronic energies. Here we show that this…
Low-dimensional ice trapped in nanocapillaries is a fascinating phenomenon and is ubiquitous in our daily lives. As a decisive factor of the confinement effect, the size of nanocapillary significantly affects the critical crystallization…
The nuclear electric quadrupole moment (NQM) of $^{87}$Sr has recently been revisited using high-precision relativistic atomic calculations [B. Lu et al., Phys. Rev. A 100, 012504 (2019)], indicating that the currently accepted value should…
Path-integral molecular dynamics simulations and electronic structure-based energy decomposition analysis (EDA) are employed to connect hydrogen bond (H-bond) strength, its asymmetry, and the total delocalization energy at the water/air…
We study the bimolecular nucleophilic substitution (S$_\mathrm{N}$2) reaction of 1-phenyl-2-trimethylsilylacetylene (PTA) under vibrational strong coupling (VSC) from the perspective of high-level ab initio quantum and polaritonic…