化学物理
We generalize the Aufbau suppressed coupled cluster formalism into the realm of doubly excited states by deriving, implementing, and testing a wave function initialization strategy that allows the zeroth order wave function to match the…
The distribution of ions and their impact on the structure of electrolyte interfaces plays an important role in many applications. Interestingly, recent experimental studies have suggested the preferential accumulation of $SO_4^{2-}$ ions…
Molecular dynamics simulations are an integral tool for studying the atomistic behavior of materials under diverse conditions. However, they can be computationally demanding in wall-clock time, especially for large systems, which limits the…
Broadband measurements of glycidaldehyde in the frequency ranges 75-170 and 500-750 GHz were recorded to extend previous analyses of its pure rotational spectrum in the microwave region. The rotational parameters of the ground vibrational…
The electronic structure calculations remain a major bottleneck in ab initio nonadiabatic molecular dynamics. We develop an efficient TDDFT-based FSSH implementation in the GPU4PySCF package for medium-sized molecular systems. Our approach…
Multiconfiguration pair-density functional theory (MC-PDFT) offers an efficient and accurate framework for computing electronic energies in strongly correlated molecular systems, with the quality of the on-top functional being a key…
Accurate prediction of adiabatic $0$-$0$ excited-state energies is crucial for modeling molecular photophysical processes. Here, we benchmark computational strategies for evaluating excited-state energies and singlet-triplet gaps obtained…
Recent reports suggest that chemical reaction rates can change when reactants are placed inside an optical cavity. These effects have been attributed to the hybridization of molecular vibrational modes with cavity modes into polaritons, but…
Machine learning interatomic potentials (MLIPs) offer first-principles accuracy with reduced computational cost, but their transferability across different thermodynamic states remains questionable, particularly for fluid systems where…
Iridium-based photosensitizers have attracted significant attention in photodynamic therapy (PDT) due to their exceptional photophysical properties and chemical stability, as well as tunable phosphorescence emission spectrum and high…
Electric field-assisted chemistry has attracted much attention in recent years, particularly in the context of oriented external electric fields for controlling molecular structure and reactivity. Such fields have been explored in a wide…
We analyse the coherent-state (CS) transformation in quantum electrodynamics coupled cluster (QED-CC) theory from the perspective of its non-vanishing commutator with the polaritonic cluster operator. Specifically, we show that a QED…
Tracking the complex non-adiabatic transitions in far-ultraviolet photodissociation demands highly accurate diabatic potential energy matrices (PEMs) across numerous excited states. To address this, we introduce a fully automated…
While human technology is ruled by determinism, biological systems exploit a subtle balance of control and stochasticity. This balance, evident in the morphogenesis of textural patterns imprinted on leaves, fur or skin can help hierarchize…
Gausslets are one of the few basis constructions for electronic structure that combine locality, orthonormality, variable resolution, and an accurate diagonal approximation for the electron-electron interaction, but the original…
The correlation discrete variable representation (CDVR) enables efficient quantum dynamics calculation with the multi-layer multi-configurational time-dependent Hartree (MCTDH) approach on general potential energy surfaces. It employs a…
We present an efficient method for rigorous quantum calculations of cross sections for atom-molecule reactive scattering in the presence of a dc electric field. The wavefunction of the reaction complex is expanded in an overcomplete set of…
Phaseless auxiliary-field quantum Monte Carlo (ph-AFQMC) has emerged as a promising electronic structure method for correlated electronic systems. However, the quality of its predictions depends critically on the choice of trial…
Machine-learned interatomic potentials (MLPs) provide near density functional theory (DFT) accuracy at reduced computational cost, but their reliability depends on representative training data and often deteriorates in transition-state…
Phaseless auxiliary-field quantum Monte Carlo (AFQMC) has in several cases been found to perform well on strongly correlated systems. Here, we benchmark the method for three iron-sulfur clusters ([2Fe-2S], [4Fe-4S], and the FeMo cofactor)…