化学物理
Zero-field (ZF) nuclear magnetic resonance (NMR) spectroscopy probes scalar J-couplings between nuclei while dispensing with large homogeneous magnetic fields, enabling low-cost and geometrically flexible detection, including through…
An iterative optimization algorithm with MD simulations in the loop is developed and applied to optimize Lennard-Jones (LJ) parameters specific for liquid tri-n-butyl phosphate (TBP). The optimization loop uses non-dominated sorting genetic…
Force fields are usually formulated directly in nuclear configuration space, whereas density functional theory is naturally formulated in terms of external potentials, densities, and variational duality. We show that exact force fields are…
Transition states, the first-order saddle points on the potential energy surfaces, govern the kinetics and mechanisms of chemical reactions and conformational changes. Locating them is challenging because transition pathways are…
Quasi-elastic neutron scattering (QENS) probes atomic and molecular motion on length and time scales central to catalysis, energy materials, and gas adsorption. However, conventional analytical fitting of QENS spectra often fails to…
Two-component linear-response time-dependent density functional theory (TDDFT) provides a unified framework that encompasses noncollinear excitations in noncollinear reference states, as well as both spin-conserving and spin-flip…
Vibrational spectroscopy provides a powerful connection between molecular dynamics (MD) simulations and experiment, but its routine use in condensed-phase systems remains limited. We introduce mimyria, a modular and automated framework that…
The ability to directly measure radiative-association rate coefficients for reactions between ions and neutral molecules has long challenged chemical physics laboratories, yet radiative association is one of the most important processes…
The study of biomolecular folding has been greatly advanced by single-molecule force spectroscopy (SMFS), which enables the observation of the dynamics of individual molecules. However, extracting quantitative models of fundamental…
Selected configuration interaction (SCI) methods are effective for treating strongly correlated electronic systems, yet their scalability has long been limited by implementations that replicate the configuration interaction (CI) vector…
Recent advances in combustion science have led to the generation of large volumes of data from high-fidelity simulations, detailed chemical-kinetic calculations and engine-relevant measurements and create new opportunities for data-driven…
Surface hopping (SH) methods are typically employed to simulate ultrafast nonadiabatic processes, but long timescales often remain beyond their reach. To address this, accelerated SH scheme mitigate this limitation by scaling the driving…
In the theory of open quantum systems, spectral densities are key quantities for modeling the dynamics and spectroscopic properties of the system under investigation. In the case of light-harvesting complexes, they encode the…
Action-detected two-dimensional electronic spectroscopy (A-2DES) could potentially be a versatile chemical tool with applicability across a range of photophysical observables such as photocurrent, photoionization, or fluorescence. However,…
Thermal conductivity of aligned polymer molecules can be exceptionally high along the alignment direction due to energy transport through strong covalent bonds. At the same time, it is highly sensitive to molecular conformation, varying by…
We present a theoretical and numerical study of the correlation between electrons and the fermionic $^{13}$C and $^{19}$F nuclei. We use the random-phase approximation (RPA) as a valuable tool in obtaining these correlation energies. A…
We introduce Suiren-1.0, a family of molecular foundation models for the accurate modeling of diverse organic systems. Suiren-1.0 comprising three specialized variants (Suiren-Base, Suiren-Dimer, and Suiren-ConfAvg) is integrated within an…
We present a methodology for accelerating the estimation of the free energy from path integral Monte Carlo simulations by considering an intermediate artificial reference system where interactions are inexpensive to evaluate numerically.…
Light-activated drugs are a promising way to treat localized diseases for which existing treatments have severe side effects. However, their development is complicated by the set of photophysical and biological properties that must be…
Machine-learning models of atomic-scale interactions achieve the accuracy of the quantum mechanical calculations on which they are trained, but at a dramatically lower computational cost. Their predictions can be made trustworthy by…