化学物理
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…
Machine learning-based simulators offer the potential to model the dynamics of complex systems more efficiently than classical approaches, while retaining differentiability, a key property for materials design. Graph neural network…
Once trained, machine-learned interatomic potentials (MLIPs) provide a fast and accurate way to study catalytic reaction pathways, but their performance strongly depends on the training set. Here, we compare nine MLIPs trained with…
The current catalyst discovery and development pipeline for energy-intensive applications like methane conversion remains bottlenecked by expensive trial-and-error experimentation, irreproducible chemical intuition, and a lack of frameworks…
Recent real-time TDDFT calculations have reported an unexpected delayed growth of molecular dipole oscillations some time after an extreme-ultraviolet (XUV) pulse is applied. We show that numerical and analytical arguments suggest that this…
The recently developed Doubles Connected Moments (DCM) expansion offers a tractable approach for computing correlation energy, exhibiting an noniterative O(N^6) scaling with system size N. Benchmark calculations on a set of molecules…
Accurate calculation of free energies and their derivatives is central to assessing the thermodynamic stability of molecular and particulate systems across length scales. Yet such quantities can be difficult to compute reliably in strongly…
Oriented external electric fields are ubiquitous in chemistry; however, the effects of fields applied in different directions on molecular systems remain underexplored. A major challenge is that an applied field exerts a torque on a…
Non-radiative decay in photoexcited molecular systems is driven by nuclear motion toward conical intersections (CIs), where electronic states become degenerate and nonadiabatic transitions occur. Identifying the nuclear degrees of freedom…
Ab initio calculations are fundamentally bottlenecked for large systems by the steep computational scaling of solving self-consistent field (SCF) equations. While machine learning offers potential accelerations, existing methods often…
Near-degenerate electronic structures remain a major challenge for conventional single-reference density functional theory (DFT). To address this problem, we propose time-dependent $\Delta$SCF (TD$\Delta$SCF), a novel linear-response scheme…
We present a deterministic optimization framework for Neural Network Quantum States (NQS) designed to bypass the sampling variance and slow mixing issues inherent in stochastic optimization. By projecting a neural backflow ansatz onto…
We present an investigation of one-photon valence-shell photoelectron spectroscopy and photoelectron circular dichroism (PECD) for the chiral molecule (1R,4R)-3-(heptafluorobutyryl)-(+)-camphor (HFC) and its europium complex Eu(III)…
Single-Hessian Gaussian wavepacket dynamics (GWD) significantly reduces the computational burden of Heller's local harmonic GWD, while maintaining comparable accuracy in approximating vibronic spectra. Here, we provide a new, symplectic…
Positron binding energies and Dyson orbitals for five-membered heterocycles with N, O, S and NH substituents are predicted \emph{ab initio} via many-body theory. The positron-molecule correlation potential (self energy) is calculated via…
Computational complexity and storage requirements are crucial factors influencing the performance and efficiency of convolutional neural networks (CNNs) in resource-constrained environments. This paper presents a high-performance embedded…
The ultrafast nonlinear optical response of molecular ensembles is fundamentally altered under strong light-matter coupling. To rigorously isolate the genuine many-body contributions, an exact time-domain field-subtraction protocol is…
Many computational methods in ab initio quantum chemistry are formulated in terms of high-order tensor contractions, whose cost determines the size of system that can be studied. We introduce stochastic tensor contraction to perform such…