化学物理
Nuclear quantum effects and non-Born--Oppenheimer effects play a vital role in many chemical and biological processes, motivating the incorporation of such effects into dynamical simulations. In real-time nuclear--electronic orbital…
The last decade has witnessed a rapid advancement in laser technology, enabling the direct monitoring and control of electronic motion on its natural attosecond to sub-femtosecond timescales. Ultrafast processes are conventionally studied…
In this work, we establish a direct connection between supplemented Dyck language and the signed expectation value of chains of second quantization operators relatively to the physical vacuum and relatively to a one-determinant state.…
This paper proposes a novel framework connecting fermionic second quantization and Dyck languages. By defining translations of creation and annihilation operators using bracket alphabets, the study establishes nullity criteria for…
We revisit the three-body problem in quantum mechanics in two and three dimensions, generating both exact eigenvalues and eigenvectors of the Hamiltonian and a series of approximate solutions as calculated with a variety of different…
While spin-adapted time-dependent density functional theory (TDDFT) approaches significantly improve the excitation energies and gradients of open-shell molecules, the effect of spin-adaptation on nonadiabatic coupling matrix elements…
Energetic-materials performance gains translate directly into reduced propellant mass, smaller warheads, and more efficient civilian gas-generators, yet no new HMX-class compound has been disclosed in fifteen years. Designing one is a…
Energy-time entangled photons provide new opportunities for controlling multiphoton absorption beyond classical limits. Here, we investigate biexciton generation in nanocrystal quantum dots driven by energy-time-entangled quantum light…
Chemistry's rules carry exceptions: the octet rule, Hess's Law, detailed balance, orbital symmetry selection rules, all with disclaimers memorised separately. Their cause: a question from a richer structural level posed in the vocabulary of…
Action-detected two-dimensional (2D) spectroscopy resolves the time-dependent nonlinear optical response of a quantum system by recording incoherently detected observables such as fluorescence, photoelectrons, or photocurrents which reflect…
Excess molar enthalpies ($H_{\text{m}}^{\text{E}}$) for iodobenzene, or 1-iodonaphthalene + heptane, + decane, + dodecane, or + tetradecane mixtures at 298.15 K and 93 kPa have been measured using a Tian-Calvet micro-calorimeter. The values…
Orbital entropies, pair entropies, and mutual information have become popular tools for analysis of strongly correlated wave functions. They can quantitatively measure how strongly an orbital participates in the electron correlation and…
Realistic physical systems are characterised by emergent interactions across multiple length and time scales, posing a significant challenge for predictive machine learning (ML) models. Most scientific ML models focus on a narrow range of…
Terahertz Kerr-effect (TKE) spectroscopy provides a time-domain optical probe of the intermolecular structural dynamics of liquids, but the measured birefringence can only be interpreted microscopically if transient molecular structure,…
Nonadiabatic molecular dynamics (NAMD) is widely used to describe hot electron relaxation and nonradiative recombination processes, but high computational costs limit its application to large supercells. Here, we implement a nonadiabatic…
Electronic friction-Langevin dynamics (EF-LD) provides an efficient framework for capturing nonadiabatic effects at solid surfaces, with particular relevance to electrochemistry and molecular electronics. In this work, we investigate…
Accurate prediction of molecular correlation energies from first principles requires resolving the {O}(N^4) electron repulsion integral (ERI) tensor. Existing graph neural network approaches to the electronic structure problem often…
Force-matched water models provide a practical route from first-principles reference data to long classical and path-integral molecular simulations. Previous flexible four-site potentials in the spirit of q-TIP4P/F showed that fitting…
NMR is uniquely endowed to analyze dynamics, with line shape and relaxation measurements covering timescales over several orders of magnitude. Further insight arises from pulse sequences like chemical exchange saturation transfer or…
Neural surrogates for molecular scattering provide a route to continuously evaluable and differentiable direct simulation Monte Carlo (DSMC) collision kernels, but a small pointwise deflection-angle error is not sufficient evidence that a…