Chemical Physics
Pericyclic reactions provide stringent tests for quantum simulations because their mechanisms are governed by orbital symmetry and involve correlated transition states. In this work, we employ the variational quantum eigensolver (VQE)…
We investigated strong-field dissociative ionization of $\mathrm{CF_2I_2}$ ensembles prepared in different initial rotational-state distributions using an electrostatic deflector. Pronounced changes in ion-channel branching ratios revealed…
Stark spectroscopy is a powerful method for probing molecular dipole moment changes, charge transfer dynamics, and polarizability under applied electric fields. Time-Resolved Terahertz Stark Spectroscopy (TRTSS), which employs intense…
Gaussian wavepacket (GWP) methods are prevalent means of solving the nuclear time-dependent Schrodinger equation (TDSE) on classical computers. They consist of representing the nuclear wave function as a superposition of Gaussians. Here, we…
In this work, we derive closed-form expressions for multi-time correlation functions underlying higher-order nonlinear spectroscopic response functions within the harmonic approximation. Our method includes displacements, frequency changes,…
The quality of multi-scale modelling techniques in molecular electronic structure calculations, such as embedding and subspace methods, relies upon the chosen active space. The automation of active space selection is vital for ensuring the…
We develop a thermodynamic theory of electric double layers in binary liquid mixtures by allowing the Stern-layer capacitance to depend on the local solvent composition. This coupling produces an additional negative contribution to the…
Simulating multidimensional quantum systems at finite temperature is inherently challenging as the system is no longer described by a single, pure-state wavefunction but by a density operator, squaring an already exponential scaling of the…
Self-consistent field real-time electronic structure methods are a powerful approach for modeling ultrafast processes but suffer from systematic errors in predicted transition energies, commonly known as peak shifting, that obscure direct…
Enhanced sampling techniques are central to the study of statistically rare events in the computer modeling and simulation of molecular phenomena. In this work, we report the development and integration of a Gaussian process model,…
A vast class of weak, millimolar-affinity molecular interactions governs cellular function, yet their quantitative characterization has remained largely beyond conventional methods. For over a century, biochemistry has worked within a…
Chemical kinetics has long inferred local molecular behaviour through the flask-and-molarity pairing, where well-mixed concentrations serve as the experimental readout. Yet many biological reactions occur in structured environments.…
In this paper, we examine transcomplex recombination RCs$^+$ + Br$^-$ $\to$ CsBr + R (R = Kr, Xe, Hg) for collision energies from 0.1 to 2.5 eV. Within the framework of the quasiclassical trajectory method on semiempirical diabatic…
The committor is the optimal reaction coordinate for a rare transition: it pinpoints the transition state and fixes the rate, and it governs events from protein folding to crystal nucleation. It minimises a Dirichlet energy, whose value at…
Proton exchange membrane water electrolysis (PEMWE) is a promising technology for harnessing intermittent renewable energy. This study experimentally investigates the degradation of PEMWE under fluctuating power supply, characterized by…
Gas-phase cluster growth by monomer addition is commonly modeled as an isothermal process. We develop a survival-limited framework in which association produces a thermally excited cluster that may dissociate before either cooling through…
Reduced density matrix functional theory (RDMFT) provides a rigorous framework for treating strong electron correlation, yet its application to periodic systems has long been hindered by two fundamental challenges: the lack of transferable…
Accelerating scientific discovery is among the most consequential applications of AI, and computational biomolecular simulation stands out as a particularly promising target within this broader effort. Coding agents promise to automate…
Conformer assignment is meaningful only when the measurement can distinguish the candidate structures. We formulate conformer spectroscopy as a measurement-model-dependent identifiability problem in which each modality defines an…
Hedin's formalism of functional derivatives is the best-known method for systematically constructing correlated electronic theories, largely due to the success of its lowest-order self-energy expansion, the $GW$ approximation. Beyond $GW$,…