化学物理
Although selected configuration interaction (SCI) algorithms can tackle much larger Hilbert spaces than the conventional full CI (FCI) method, the scaling of their computational cost with respect to the system size remains inherently…
A dynamical rearrangement in the electronic structure of a molecule can be driven by different phenomena, including nuclear motion, electronic coherence or electron correlation. Recording such electronic dynamics and identifying their fate…
Atomistic simulations are a powerful tool for studying the dynamics of molecules, proteins, and materials on wide time and length scales. Their reliability and predictiveness, however, depend directly on the accuracy of the underlying…
Density Functional Theory (DFT) is the de facto workhorse for large-scale electronic structure calculations in chemistry and materials science. While plane-wave DFT implementations remain the most widely used, real-space DFT provides…
We present a reformulation of QM/MM as a fully quantum mechanical theory of interacting subsystems, all treated at the level of density functional theory (DFT). For the MM subsystem, which lacks orbitals, we assign an ad hoc electron…
Nonadiabatic coupling between electrons and molecular motion at metal surfaces leads to energy dissipation and dynamical steering effects during chemical surface dynamics. We present a theoretical approach to the scattering of molecules…
Computationally tractable and reliable, albeit approximate, methods for studying exciton transport in molecular aggregates immersed in structured bosonic environments have been actively developed. Going beyond the lowest-order (Born)…
Molecular chirality has traditionally been viewed as a binary property where a molecule is classified as either chiral or achiral, yet in the recent decades mathematical methods for quantifying chirality have been explored. Here we use toy…
Predicting the exact many-body quantum dynamics of polarons in materials with strong carrier-phonon interactions presents a fundamental challenge, often necessitating one to adopt approximations that sacrifice the ability to predict the…
To date, computational methods for modeling defects (vacancies, adsorbates, etc.) rely on periodic supercells in which the defect is far enough from its repeated image such that they can be assumed non-interacting. Yet, the relative…
Accurate approximation of the exchange-correlation (XC) energy in density functional theory (DFT) calculations is essential for reliably modelling electronic systems. Many such approximations are developed from models of the XC hole;…
Two-photon fluorescence imaging has shown a promising application in biomedical imaging due to its outstanding advantages such as large penetration depth, low photo-damage, and photo-bleaching, etc. Among them, the two-photon fluorescent…
Time-dependent density-functional theory (TDDFT) is deemed to be a formally rigorous way of dealing with the time-evolution of a many-electron system at the level of electron densities rather than the underlying wavefunctions, which in turn…
Double excitations are crucial to understanding numerous chemical, physical, and biological processes, but accurately predicting them remains a challenge. In this work, we explore the particle-particle random phase approximation (ppRPA) as…
Dipole-bound states in anions exist when a polar neutral core binds an electron in a diffuse orbital through charge--dipole interaction. Electronically excited polar neutral cores can also bind an electron in a diffuse orbital to form…
Understanding the evolution of electrified solid-liquid interfaces during electrochemical reactions is crucial. However, capturing the dynamic behavior of the interfaces with high temporal resolution and accuracy over long timescales…
We present results and discuss methods for computing the melting temperature of dense molecular hydrogen using a machine learned model trained on quantum Monte Carlo data. In this newly trained model, we emphasize the importance of accurate…
Molecular optimization, which aims to discover improved molecules from a vast chemical search space, is a critical step in chemical development. Various artificial intelligence technologies have demonstrated high effectiveness and…
MnxOy coated over TiO2 nanotube array substrate was doped with Mo and polyaniline (PANI) and applied for electrochemical desulfurization of concentrated sulfide (HS) solutions at basic pH, typical of biogas scrubbing solutions and…
Chemiresistive materials, which alter their electrical resistance in response to interactions with surrounding chemicals, are valued for their robustness, rapid detection ability and high sensitivity. Recent research has revealed that the…