化学物理
Transforming rovibronic Hamiltonians of molecular systems from the $\Lambda S$ (Hund's case a) basis to the adiabatic $\Omega$ representation is widely used to "remove" spin-orbit coupling (SOC) and enable single-state treatments of spectra…
Simulating the dynamics of molecular excitons in complex nanophotonic environments requires integrating rigorous electromagnetic simulations with accurate treatments of open quantum system dynamics. In this work, we develop MQED-QD…
We present a simple relativistic exact 2-component (X2C) Hamiltonian that models two-electron picture-change effects using Lehtola's superposition of atomic potentials (SAP) [S. Lehtola, J. Chem. Theory Comput. 15, 1593-1604 (2019)]. The…
Fromager and Lasorne [Electron. Struct. 6 025002 (2024)] have recently derived an in-principle exact Kohn-Sham density functional theory (KS-DFT) of electrons and nuclei, where the nuclear density and the (so-called conditional) electronic…
We show how a spin polarization can be generated through the photo-induced electron transfer of an achiral donor-acceptor complex following chiral light excitation. In particular, we illustrate the basic energetic and symmetry requirements…
Electron transfer (ET) at electrochemical interfaces is central to energy conversion and storage, yet its theoretical and computational modeling remain active research areas. This review elucidates key concepts and theories of ET kinetics,…
Machine-learned interatomic potentials (MLIPs) have shown significant promise in predicting infrared spectra with high fidelity. However, the absence of general-purpose MLIPs that simultaneously span broad chemical diversity and provide…
Exciton transport in molecular aggregates with magic-angle orientation is expected to be strongly suppressed due to their negligible dipole-dipole interactions. However, recent reports show that light-matter interactions can significantly…
Placing an organic material on top of a Bragg mirror can significantly enhance exciton transport. Such enhancement has been attributed to strong coupling between the evanescent Bloch surface waves (BSW) on the mirror, and the excitons in…
Structure determination by chemical-shift-driven NMR crystallography relies on comparing chemical shieldings measured in solid-state NMR experiments with simulations. However, computational cost limits the accuracy of shielding predictions,…
Photoexcitation is an inherent part of any photochemical or spectroscopic experiment, yet its impact on the excited-state dynamics is often overlooked. However, it is the excited molecular state, built upon photoexcitation and shaped by the…
Electron-electron scattering is one of the most important hot carrier relaxation pathways in plasmonic nanoparticles. Understanding the dynamics of this scattering process and the effects of this on excited state dephasing and relaxation is…
A reaction-coordinate--resolved information-theoretic analysis of chemical reactivity is developed using mutual information and partial information decomposition (PID). Along an intrinsic reaction coordinate (IRC), a local empirical…
The advent of neural-network-based deep learning techniques has led to the emergence of increasingly sophisticated numerical interatomic potentials, including graph neural networks and large language-motivated foundation models.…
Despite continuing hype about the role of AI in drug discovery, no "AI-discovered drugs" have so far received regulatory approval. Here we assess one of the latest AI based tools in this domain. The ability to rapidly predict protein-ligand…
Sampling molecular conformations from the Boltzmann distribution is essential for computational chemistry, but iterative diffusion methods are prohibitively slow. Drifting Models offer one-step generation, yet their equilibrium matches the…
Chemical reaction engineering is key to industrial might and sustainable chemistry. This will be enabled using smart, efficient catalysts or catalysis ecosystems. This is possible with advanced artificial intelligence and machine learning…
Deep learning, a subfield of machine learning, has gained importance in various application areas in recent years. Its growing popularity has led it to enter the natural sciences as well. This has created the need for molecular…
We introduce a data-driven framework for approximating the convex set of $N$-representable two-electron reduced density matrices (2-RDMs). Traditional approaches characterize this set through linear matrix inequalities that define its…
Molecular simulations are widely regarded as leading candidates to demonstrate quantum advantage--defined as the point at which quantum methods surpass classical approaches in either accuracy or scale. Yet the qubit counts and error rates…