化学物理
Coarse-grained (CG) molecular dynamics simulations extend the length and time scale of atomistic simulations by replacing groups of correlated atoms with CG beads. Machine-learned coarse-graining (MLCG) has recently emerged as a promising…
Nanoalloys offer a unique opportunity to tailor chemical properties through changes in composition, shape, and size. However, this flexibility introduces complexity that challenges both experimental and conventional theoretical methods. In…
We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard X-ray scattering. Time-resolved X-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the…
Given the power of large language and large vision models, it is of profound and fundamental interest to ask if a foundational model based on data and parameter scaling laws and pre-training strategies is possible for learned simulations of…
In this tutorial we discuss the chemical potential of ions in water (i.e., in a salt solution, in an electrolyte phase) and inside (charged) nanoporous materials such as porous membranes. In water treatment, such membranes are often used to…
We demonstrate the feasibility of quantum computing for large-scale, realistic chemical systems through the development of a new interface using a quantum circuit simulator and CP2K, a highly efficient first-principles calculation software.…
Wetting of solid surfaces by a liquid is important for many natural and industrial processes such as printing, painting and coating. However, a quantitative description of the dynamic receding and advancing contact angle is still debated,…
Polaritons have gained significant attention for the tantalizing possibility of modifying chemical properties and dynamics by coupling molecules to resonant cavity modes to create hybrid light-matter quantum states. Herein, we implement the…
We develop the theory justifying the application of the density-based basis-set correction (DBBSC) method to double-hybrid approximations in order to accelerate their basis convergence. We show that, for the oneparameter double hybrids…
We propose a novel wave function partitioning method that integrates deep-learning variational Monte Carlo with ans\"atze based on generalized product functions. This approach effectively separates electronic wave functions (WFs) into…
At an electrode, water molecules align to the surface field upon voltage application. This initiates important electrochemical reactions, e.g., hydrogen and oxygen evolution reactions. Recently developed non-linear optical techniques…
We present constrained random walk (cRW) and figure of merit (FOM) based non-linear optimization procedures for systematic design and fundamental understanding of magnetic resonance experiments dressing bilinear and linear effective…
Sampling strategies in diffusion models are critical to molecular generation yet remain relatively underexplored. In this work, we investigate a broad spectrum of sampling methods beyond conventional defaults and reveal that sampling choice…
Singlet fission, a phenomenon in which a singlet exciton is converted to two triplet excitons, is sensitive to vibrations that perturb couplings between electronic states (i.e., Peierls vibrations). In singlet fission models larger than…
In this study, we employ the variational quantum eigensolver algorithm with a multireference unitary coupled cluster ansatz to report the ground state energy of the BeH2 molecule in a geometry where strong correlation effects are…
We introduce the Vector-QM24 (VQM24) dataset comprehensively covering all possible neutral closed-shell small organic and inorganic molecules with up to five heavy (\textit{p}-block) atoms: C, N, O, F, Si, P, S, Cl, Br. All valid…
We present the quantum-selected configuration interaction-tailored coupled-cluster (QSCI-TCC) method, a hybrid quantum-classical scheme that tailors coupled-cluster (CC) theory with a quantum-selected configuration interaction (QSCI) wave…
Proton-coupled electron transfers (PCET) are elementary steps in electrocatalysis. However, accurate calculations of PCET rates remain challenging, especially considering nuclear quantum effects (NQEs) under a constant potential condition.…
We investigate the ability of Aufbau suppressed coupled cluster theory to act as a post-linear-response correction to widely used linear response methods for electronically excited states. We find that the theory is highly resilient to…
Leveraging matrix sparsity has proven a fruitful strategy for accelerating quantum chemical calculations. Here we present the hierarchical SOS-MP2 algorithm, which uses hierarchical matrix ($\mathcal{H}^{2}$) compression of the electron…