化学物理

Recent advances in occupancy extrapolation (OE) show that potential of orbital-occupation based energy functions can describe electronic excitations. Here, the OE method in the particle-hole channel is extended to an effective quasiparticle…

We present a Bethe-Salpeter equation (BSE) solver based on a self-consistent $GW$ reference evaluated on the Matsubara frequency axis, referred to as BSE@sc$GW$. The self-consistent $GW$ starting point provides a robust quasiparticle…

We introduce a new equation-of-motion coupled-cluster method based on a pair coupled-cluster doubles (pCCD) reference, termed frozen-pair EOM-CCSD (EOM-fpCCSD). This approach combines the computational efficiency of the pCCD ansatz with a…

Exciton transfer dynamics between chromophores depends on excitonic coupling, which is governed by relative orientation between the chromophores. While the excitonic coupling is treated as a static parameter in many cases, structural…

Reaction-diffusion processes play an important role in a variety of physical, chemical, and biological systems. Conventionally, the kinetics of these processes are described by the law of mass action. However, there are various cases where…

Coarse-graining (CG) reduces molecular details to extend the time and length scales of molecular dynamics simulations to microseconds and micrometers. However, the CG approaches have long been limited by the difficulty of constructing both…

Photosynthesis relies on efficient energy relaxation within the excited-state manifold of pigment-protein complexes. Since the protein scaffold is rather flexible, the resulting energetic and structural disorder gives rise to a complex…

An 11-species thermochemical model for H$_2$/ He mixtures with state-specific kinetics for atomic H is developed and used to simulate 1-D shocks at conditions relevant for ice and gas giant entry flows. To implement this kinetic model, a…

Excited-state electronic structure in strongly correlated systems remains challenging due to the exponential scaling of the many-body Hilbert space and the difficulty of constructing systematically controlled active spaces. Building on the…

We assess the performance of the Quantum Flow (QFlow) algorithm employing cost-effective solvers based on the unitary coupled-cluster ansatz with single and double excitations (QFlow-SD). The resulting energies are benchmarked against those…

Asymmetric valences in a binary electrolyte can significantly affect the performance of systems such as reverse electrodialysis cells, batteries, and supercapacitors. To generate a theoretical understanding of this effect, we consider a…

We present a class and home problem in graduate transport phenomena and electrochemical engineering that clarifies a common misconception: electroneutrality implies the electric field is constant. Starting with one-dimensional…

We present a combined imaginary-time/real-time time-dependent (TD) approach for evaluating linear absorption spectra of open-shell systems at the electron attachment (EA) and ionization potential (IP) equation-of-motion coupled-cluster…

We present OmniMol, a state-of-the-art all-to-all transformer-based small molecule machine-learned interatomic potential (MLIP). OmniMol is built by adapting Omnilearned, a foundation model for particle jets found in high-energy physics…

The functional properties of photoactive proteins are governed by the interplay between bright and dark excited states. While the bright states are well-studied, the dark states, which are fundamental to photostability and light harvesting,…

Tandem catalysis involves two or more catalysts arranged in proximity within a single reaction vessel, with the aim of synergistically aligning the catalysts' reaction pathways to maximize overall system performance. This study presents a…

The implicit solvent approach offers a computationally efficient framework to model solvation effects in molecular simulations. However, its accuracy often falls short compared to explicit solvent models, limiting its use in precise…

We revive an approach to solve the Dirac equation originally proposed by Kutzelnigg which makes use of the squared Dirac operator $\hat{\mathfrak{D}}^{2}$. This approach holds the promise to avoid the negative energy solution because the…

Matsubara dynamics is the classical dynamics which results when imaginary-time path-integrals are smoothed; it conserves the quantum Boltzmann distribution and appears in drastically approximated form in path-integral dynamics methods such…

In this work, we report on the high-resolution infrared spectrum of CCH$^+$ ($^3\Pi$) recorded in the range $3066-3184$~cm$^{-1}$ by means of leak-out spectroscopy. This spectral range covers the fundamental of the CH stretching mode and a…