化学物理
We develop a unified quantum geometric framework to understand reactive quantum dynamics. The critical roles of the quantum geometry of adiabatic electronic states in both adiabatic and non-adiabatic quantum dynamics are unveiled. A…
The nonlocal dielectric properties of liquid water are studied in the context of {\it ab initio} molecular dynamics simulations based on density functional theory. We calculate the dielectric response from the charge structure factor of the…
We investigate the intrinsic behavior of ionic liquids under shear flow, using a coarse-grained model of C4mim-PF6 as a prototypical example. The importance of long-ranged electrostatics is assessed as a function of shear rate by comparing…
Ionic transport within charged nanopores is commonly represented by resistor-capacitor transmission line circuits, where charging electrical double layers are modeled as capacitors, and the resistance to ionic current is modeled as…
Orbital entropies, pair entropies, and mutual information have become popular tools for analysis of strongly correlated wave functions. They can quantitatively measure how strongly an orbital (e.g. from the DMRG active space) participates…
Molecular dynamics (MD) simulations play a crucial role in resolving the underlying conformational dynamics of molecular systems. However, their capability to correctly reproduce and predict dynamics in agreement with experiments is limited…
Neural Networks (NNs) are effective models for refining the accuracy of molecular dynamics, opening up new fields of application. Typically trained bottom-up, atomistic NN potential models can reach first-principle accuracy, while…
Calculations of highly excited and delocalized molecular vibrational states are computationally challenging tasks, which strongly depends on the choice of coordinates for describing vibrational motions. We introduce a new method that…
Thermally activated delayed fluorescence (TADF) offers the promise of highly efficient organic light emitting diodes (OLEDs), without the heavy metals requirement of the previous generation of OLEDs. However, the design of new TADF emitters…
The fundamental non-Hermitian nature of the forms of coupled-cluster (CC) theory widely used in quantum chemistry has usually been viewed as a negative, but the present letter shows how this can be used to advantage. Specifically, the…
Polaritonic chemistry offers the possibility of modifying molecular properties and even influencing chemical reactivity through strong coupling between vibrational transitions and confined light modes in optical cavities. Despite…
Machine learning potentials (MLPs) have become a popular tool in chemistry and materials science as they combine the accuracy of electronic structure calculations with the high computational efficiency of analytic potentials. MLPs are…
Hydrogen bonding is an important non-covalent interaction that plays a major role in molecular self-organization and supramolecular structures. It can be described accurately with ab initio quantum chemical wave function methods, which…
Vibrational polaritons, hybrid light-matter states formed between molecular vibrations and infrared (IR) cavity modes, provide a novel approach for modifying chemical reaction pathways and energy transfer processes. For vibrational…
Recent experiments have demonstrated that polariton formation provides a novel strategy for modifying local molecular processes when a large ensemble of molecules is confined within an optical cavity. Herein, a numerical strategy based on…
Diffusion models have emerged as powerful tools for molecular generation, particularly in the context of 3D molecular structures. Inspired by non-equilibrium statistical physics, these models can generate 3D molecular structures with…
Large language models (LLMs) can perform accurate classification with zero or few examples through in-context learning. We extend this capability to regression with uncertainty estimation using frozen LLMs (e.g., GPT-3.5, Gemini), enabling…
The software package DIALECT is introduced, which provides the capability of calculating excited-state properties and nonadiabatic dynamics of large molecular systems and can be applied to simulate energy and charge-transfer processes in…
SpectraMatcher is a cross-platform desktop application for interactive comparison of experimental and computed vibronic spectra, designed to assist in the recognition and assignment of spectral patterns. It provides an intuitive graphical…
The combination of isochoric heating of solids by free electron lasers (FEL) and in situ diagnostics by X-ray Thomson scattering (XRTS) allows for measurements of material properties at warm dense matter (WDM) conditions relevant for…