化学物理
Practical applications of fragment embedding and closely related local correlation methods critically depend on a judicious choice of a low-level theory to define the local embedding subspace and to capture long-range electrostatic and…
The planar to Dewar valence isomerisation of 4a,8a-azaboranaphthalene (BN$_\text{Naph}$), a $\pi$ extended BN-doped analogue of azaborine, is investigated to evaluate how BN incorporation reshapes the minimum energy pathway on the ground…
We introduce two-quantum (2Q) fluorescence-detected pump-probe (F-PP) spectroscopy as a tool to probe ultrafast multiparticle interactions in many-body systems. We describe a pulse-shaper-based fully collinear setup utilizing phase cycling…
Ammonia has strong poisoning effects on cathode catalyst layers of proton exchange membrane (PEM) fuel cells, but the poisoning mechanism is still unclear. In this study, all-atom molecular dynamics simulations are employed to investigate…
Geometrical imperfections in quadrupole mass filters introduce higher-order field components that can significantly influence device performance, particularly under non-sinusoidal excitation. In this work, a comprehensive simulation study…
Cementitious materials are widely used for hazardous-waste encapsulation, yet the molecular mechanisms governing heavy-metal ion retention across different gel chemistries remain insufficiently resolved. Here, classical molecular dynamics…
We present an efficient implementation of a one-step relativistic second-order multireference perturbation theory based on the multireference driven similarity renormalization group (MR-DSRG) using the exact two-component (X2C) Hamiltonian,…
In this work, we develop a size extensive Auxiliary-Field Quantum Monte Carlo (AFQMC) approach that scales as $O(N^5)$ for local energy evaluation by treating the Coupled Cluster Singles and Doubles (CCSD) trial wavefunctions…
The homogeneous spectral linewidth associated with light-matter interactions is a fundamental descriptor of the optical properties of materials, governed by the quantum dynamics of the condensed-matter system. We discuss here that the…
The parameterization of simulation-based models is a central yet laborious task in computational chemistry and physics, often driven by human intuition and manual iteration. Automating this task necessitates the definition of suitable…
Relative Binding Free Energy (RBFE) calculations are a cornerstone of rational hit-to-lead and lead optimization in modern drug discovery. However, the high computational cost and limited reliability in tackling large or complex molecular…
Quantum computing offers the promise of revolutionizing quantum chemistry by enabling the solution of chemical problems for substantially less computational cost. While most demonstrations of quantum computation to date have focused on…
Null points in synthetically tunable molecular aggregates are predicted to generate flat energy bands analogous to those known in strongly correlated condensed-matter physics. For chemistry, null points provide a powerful design principle…
Nuclear magnetic resonance (NMR) spectroscopy provides an experimental readout of local chemical environments, but its use in molecular representation learning has been constrained by heterogeneous data and incomplete atom-level…
The accurate description of electron correlation is a central challenge in computational chemistry, with selected configuration interaction (SCI) emerging as a powerful tool to approach the full CI limit. While recent machine learning (ML)…
We study a simple but useful test for neural exchange-correlation (XC) functionals: can a neural model reproduce an established XC functional when it is used self-consistently? We call this test functional cloning. The model is trained at…
In density functional theory, simpler exchange-correlation (XC) approximations such as the local density approximation (LDA) are favored for computational speed but rely on limited information, leading to a trade-off between accuracy and…
The nuclear Schiff interaction (NSI) arises from a nuclear force that simultaneously violates spatial parity (P) and time reversal (T) symmetries, where T symmetry is equivalent to CP symmetry under CPT invariance. Detecting the NSI…
We study steady-state resonance light scattering from ensembles of noninteracting molecules, both in free space and inside optical cavities, while accounting for local thermal relaxation. The scattering spectra are obtained from…
A general polarizable embedded (PE) quantum mechanics/molecular mechanics scheme for periodic systems is presented, describing mutual polarization of the two subsystems. The QM system, described with density functional theory (DFT), is…