化学物理
Understanding ion adsorption at electrified metal-electrolyte interfaces is essential for accurate modeling of electrochemical systems. Here, we systematically investigate the free energy profiles of Na$^+$, Cl$^-$, and F$^-$ ions at the…
Computing excited states of many-body quantum Hamiltonians is a fundamental challenge in computational physics and chemistry, with state-of-the-art methods broadly classified into variational (critical point search) and linear response…
Van der Waals (vdW) interactions are essential for describing molecules and materials, from drug design and catalysis to battery applications. These omnipresent interactions must also be accurately included in machine-learned force fields.…
In this work, we have studied the effect of base-pairing on the shape resonances of guanine and cytosine nucleobases. Among the seven {\pi}* resonances we identified in the guanine-cytosine (GC) anion radical, three were centered on…
A discrete binomial random-walk description of molecular collisions is used to quantify the variance of coarse-grained velocity fields arising solely from collision-induced momentum exchange. Closed-form expressions for the growth of…
We report a set of adiabatic potential energy surfaces (PESs) for diiodomethane, including the ground electronic state and all excited states accessible via single-photon absorption near 260 nm. Although constrained to four dimensions,…
We present an efficient theoretical model to simulate observables in the time-resolved coincident three-ion Coulomb explosion experiment of diiodomethane. The model employs two degrees of freedom to describe the C-I bond breaking and the…
Fluids in nanopores are of importance for many engineering applications, including energy storage in supercapacitors, hydrocarbons recovery from unconventional sources, or water desalination. Thermodynamic properties of fluids confined in…
Protein electrostatics tune excitation energies in the Photosystem II reaction center (PSII-RC), yet a fully quantum-mechanical many-body description of how the surrounding protein environment renormalizes excitons has remained…
Machine-learned interatomic potentials enable large systems to be simulated for long time scales at near ab-initio accuracy. This accuracy is achieved by fitting extremely flexible model architectures to high quality reference data. In…
Attosecond science is an emerging topic where chirality plays a central role. Here we demonstrate subjecting iodoacetylene, a geometrically achiral molecule, to a pair of simulated non-ionizing ultrafast circularly polarized laser pulses at…
We report an iterative algorithm to retrieve accurate real space information from gas phase ultrafast diffraction measurements with missing data at low momentum transfer. The algorithm operates in a manner similar to phase retrieval…
Multiscale simulations facilitate the efficient exploration of large spatiotemporal scales in chemical and physical systems, yet particle-based simulations become prohibitively expensive at time and length scales beyond the molecular level.…
Accurate molecular property predictions require 3D geometries, which are typically obtained using expensive methods such as density functional theory (DFT). Here, we attempt to obtain molecular geometries by relying solely on machine…
We report the potential energy curve, the diagonal Born-Oppenheimer, non-adiabatic mass, relativistic, and leading-order QED corrections for the ground electronic state of the helium dimer cation; the higher-order QED and finite-nuclear…
A potential energy curve (PEC) accurate to a fraction of 1 ppm ($1:10^6$) is computed for the $^3\Sigma_\mathrm{u}^+$ state of He$_2$ endowed with relativistic and QED corrections. The nuclear Schr\"odinger equation is solved on this PEC…
We present a reduced density operator for electronically open molecules by explicitly averaging over the environmental degrees of freedom of the composite Hamiltonian. Specifically, we include the particle-number non-conserving…
Metal halide perovskites (MHPs) have attracted significant attention owing to their simple manufacturing process and unique optoelectronic properties. Their reversible electrical or optical properties changes in response to oxidizing or…
Organic molecular crystals underpin technologies ranging from pharmaceuticals to organic electronics, yet predicting solid-state packing of molecules remains challenging because candidate generation is combinatorial and stability is only…
Accurate simulations of molecules require high-level electronic-structure theory in combination with rigorous methods for approximating the quantum dynamics. Machine-learning approaches can significantly reduce the computational expense of…