化学物理
$\Lambda$-doubling of diatomic molecules is a subtle microscopic phenomenon that has long attracted the attention of experimental groups, insofar as rotation of molecular $\textit{nuclei}$ induces small energetic changes in the (degenerate)…
This paper extends the previously reported theory of dissipation pathways [J. Chem. Phys. 160, 214111 (2024)] to incorporate off-diagonal subsystem-bath coupling, which is often required to model molecular systems where the environment…
Molecular dynamics (MD) provides insights into atomic-scale processes by integrating over time the equations that describe the motion of atoms under the action of interatomic forces. Machine learning models have substantially accelerated MD…
In this work, we present Enhanced Representation-Based Sampling (ERBS), a novel enhanced sampling method designed to generate structurally diverse training datasets for machine-learned interatomic potentials. ERBS automatically identifies…
On-surface synthesis has allowed for the tuneable preparation of numerous molecular systems with variable properties. Recently, we demonstrated the highly selective synthesis of kekulene (>99%) on Cu(111) and isokekulene (92%) on Cu(110)…
Optimal tuning of functional parameters in density functional theory approximations, based on enforcing the ionization potential theorem, has emerged as the method of choice for the non-empirical prediction of the electronic structure of…
Typical path integral Monte Carlo approaches use the primitive approximation to compute the probability density for a given path. In this work, we develop the pair Discrete Variable Representation (pair-DVR) approach to study molecular…
In this work, we propose a Path Integral Monte Carlo (PIMC) approach based on discretized continuous degrees of freedom and rejection-free Gibbs sampling. The ground state properties of a chain of planar rotors with dipole-dipole…
We study light-mediated interactions between spatially separated molecules using real-time quantum electrodynamical time-dependent density functional theory based on the Pauli-Fierz Hamiltonian. An ultrashort delta-kick excitation…
Ten high resolution Fourier transform spectra of the pentad region near 3.3 {\mu}m of methane diluted in carbon dioxide at total pressures up to 800 hPa have been recorded at 296.5(5) K. Including a high resolution spectrum of pure methane…
Molecular dynamics (MD) simulations are a central tool in science and engineering enabling the study of dynamical behavior and the link between microscopic structure and macroscopic function. Their high computational cost, however, has…
Gas phase ultrafast electron diffraction (GUED) has become a powerful technique to directly observe the structural dynamics of photoexcited molecules. GUED reveals information about the nuclear motions that is complementary to the…
The small magnitude and long-range character of non-covalent interactions pose a significant challenge for computational quantum chemical and electronic-structure methods alike. State-of-the-art coupled cluster (CC) theory and…
Understanding the relationship between molecular structure and chemical reactivity or properties is fundamental to rational molecular design. Linear free energy relationships (LFERs), particularly Hammett analysis, have long served as…
Harnessing strong light-matter interactions to control chemical reactions in confined electromagnetic fields offers a promising route toward deepening our understanding of chemical dynamics at the collective quantum-mechanical level, with…
Plasmonic nanoparticles generate strongly localized and enhanced light field through localized surface plasmon resonance, thereby playing a central role in plasmonics and nanophotonics. Because the optical properties of plasmonic…
The design-make-test-analyze cycle in early-stage drug discovery remains constrained primarily by the "make" step: small-molecule synthesis is slow, costly, and difficult to scale or automate across diverse chemotypes. Enumerated chemical…
Modern cryopreservation exists at the convergence of diverse disciplines--materials science, physical chemistry, mechanical engineering, biological engineering, etc.--and emerging technologies often draw from many of these disciplines…
Predicting non-covalent host-guest recognition remains challenging due to the complex interplay of electrostatics, dispersion, and steric effects, and the limited transferability of existing docking approaches to synthetic supramolecular…
Branching ratios for fragmentation channels of important meta- and unstable species are essential for a molecular-level characterization of atmospheric chemistry. Here, the molecular product channels for the decomposition dynamics of the…