化学物理
Slater determinants have underpinned quantum chemistry for nearly a century, yet their full potential has remained challenging to exploit. In this work, we show that a variational wavefunction composed of a few hundred optimized…
In this paper, we develop a class of antisymmetrized geminal power configuration interaction (AGP-CI) wave functions that extend the AGP framework by incorporating inter-geminal correlations through a CI expansion. To make these…
The computation of excited states within the Complete Active Space Self-Consistent Field (CASSCF) framework remains a significant challenge in quantum chemistry, both theoretically and algorithmically. In this work, we extend the K\"ahler…
We introduce a simulation technique to compute the free energy difference between two hydrate structures of different stoichiometry connected to a reservoir of gas molecules at a prescribed pressure. The method permits the determination of…
We present an efficient implementation of the low-cost linear-response coupled-cluster singles and doubles (LR-CCSD) method for computing static and frequency-dependent polarizabilities in systems with significant relativistic and…
Gas hydrates are potential candidates in future energy sources while simultaneously providing structures with extensive applications in carbon capture and storage, gas transport, and important separation processes. Prior research in the…
Transferable excited-state dynamics offer a route to efficient screening of photophysical behavior across molecular systems, but conventional nonadiabatic simulations remain prohibitively expensive. Here we introduce X-MACE, a transferable…
A path-integral hybrid Monte Carlo approach with enveloping bridging potentials (PIHMC-EBP) is proposed for calculating numerically exact tunneling splittings in molecular systems. The central idea is to construct an approximately…
We extend our previous symmetrized path-integral molecular dynamics approach to calculate tunneling splittings of molecules in rotationally excited states. In this new formalism, the system is rigorously projected onto selected rotational…
The theory of hyper-Rayleigh scattering optical activity (HRS-OA) spectroscopy has previously been described within the length formulation of the pure electric-dipole and mixed (electric-dipole/magnetic-dipole and…
The interest to foster plasmonic applications at energies in the ultra-violet, has escalated research initiatives in clusters of unconventional plasmonic materials like aluminum and indium,for which the surface-plasmon resonance appears…
Machine learning is revolutionizing chemistry. Beyond the value of predictive models accelerating virtual screening, generative AI aims at enabling inverse design, reversing the compound-to-property prediction paradigm into…
We derive analytical nuclear gradients for state-averaged orbital-optimized configuration interaction singles (SACIS) and its spin-projected extension (SAECIS), enabling efficient geometry optimization and minimum-energy conical…
Quantum chemistry is a foundational enabling tool for the fields of chemistry, materials science, computational biology and others. Despite of its power, the practical application of quantum chemistry simulations remains in the hands of…
Capturing the structural changes that molecules undergo during chemical reactions in real space and time is a long-standing dream and an essential prerequisite for understanding and ultimately controlling femtochemistry. A key approach to…
The wettability of monolayer and multilayer graphene remains a topic of longstanding debate. Here, we combined first-principles molecular dynamics simulations accelerated with the atomic cluster expansion machine learning interatomic…
Ground-state electronic structure calculations using Kohn-Sham density functional theory (KS-DFT) offer an unprecedented balance between efficiency and accuracy, now paradigmatic to the fields of quantum chemistry and condensed matter…
We simulate a third-order nonlinear signal in a pump-probe spectroscopy from the interference between first- and second-order wavepackets (WPs), as well as from a state-to-state transition for Stokes and coherent anti-Stokes pathways in the…
We present a computational platform for modeling chemical reactions in complex molecular environments, focused on ligand-protein binding in drug discovery. The platform implements our new quantum-in-quantum-in-classical (QM/QM/MM)…
To further develop accurate and large-scale simulations of electrochemical interfaces, we propose a unified explicit electric potential framework to simultaneously predict atomic forces and electron density distributions. The framework…