Chemical Physics
For decades, scientists have studied the intricate charge migration dynamics, where after ionization a localized charge distribution ("hole") migrates across the molecule on a femtosecond timescale. This has the potential for controlling…
A comparison of the {\it ab initio} calculations using the i-DMFT Method by Di Liu et al. (2025) with benchmark potential curves for three HX(F,Cl,Br) halides shows their inaccuracy in the domain around equilibrium - they do not reproduce…
We outline the design and characterization of a laser pulse shaper, which creates an ``ultraslow optical centrifuge'' - a linearly polarized field whose polarization vector rotates with arbitrarily low angular acceleration. By directly…
Molecular structure elucidation from spectroscopic data is a long-standing challenge in Chemistry, traditionally requiring expert interpretation. We introduce NMIRacle, a two-stage generative framework that builds upon recent paradigms in…
Understanding the mechanism of chemical reaction rate modulation by vibrational strong coupling (VSC) has been the focus of several recent studies. However, a definitive explanation for the mode-specificity of VSC still eludes us. In this…
We use optical-optical double-resonance (OODR) spectroscopy to measure for the first time hot-band transitions of ethylene (C${_2}$H${_4}$) between states in the 3000 cm$^{-1}$ and 9000 cm$^{-1}$ energy ranges. A 3.2 ${\mu}$m continuous…
Collective light-matter systems host an extensive manifold of dark states whose role in the emergence of thermodynamic behavior remains poorly understood, especially in the presence of disorder and structured environments. Here, we develop…
We use sub-Doppler optical-optical double-resonance (OODR) spectroscopy with a 3.3 ${\mu}$m single-frequency pump and a cavity-enhanced 1.65 ${\mu}$m comb probe to measure 33 ladder-type (3${\nu}$${_3}$ ${\leftarrow}$ ${\nu}$${_3}$) and 8…
The generation of unidirectional motion has been a long-standing challenge in engineering of molecular motors. Here, a mechanism driving the rotation is presented based on electron current through helical orbitals on a $\pi$-bonded carbon…
Hyperpolarisation using Signal Amplification By Reversible Exchange (SABRE) is a convenient method for high repeatability studies. The core of this technique is polarisation transfer to the target substrate during an on-going chemical…
Excited atoms and molecules can utilize their excess energy to ionize a neighboring system by a process named interatomic and intermolecular Coulombic decay (ICD). ICD is ultrafast, in the femtosecond regime, and has many modes of…
We define and calculate the triplet-pair population of the $2^1A_g$ dark state in polyenes, as predicted by the $\pi$-electron Pariser-Parr-Pople (PPP) model, for chains of 8 to 14 C-atoms and Coulomb interaction parameter between 4-14 eV.…
We compute highly accurate first principle based \textit{ab initio} adiabatic potential energy surfaces (PESs) using State-Averaged Multi-Configurational Self-Consistent Field (SA-MCSCF) followed by internally contracted Multi-Reference…
Quantitative prediction of thermodynamic properties in solution is essential for translating atomistic simulations into reliable chemical insight. As an exemplar system, the behaviour of CaCO$_3$ in water has been widely studied to…
Transforming rovibronic Hamiltonians of molecular systems from the $\Lambda S$ (Hund's case a) basis to the adiabatic $\Omega$ representation is widely used to "remove" spin-orbit coupling (SOC) and enable single-state treatments of spectra…
Simulating the dynamics of molecular excitons in complex nanophotonic environments requires integrating rigorous electromagnetic simulations with accurate treatments of open quantum system dynamics. In this work, we develop MQED-QD…
We present a simple relativistic exact 2-component (X2C) Hamiltonian that models two-electron picture-change effects using Lehtola's superposition of atomic potentials (SAP) [S. Lehtola, J. Chem. Theory Comput. 15, 1593-1604 (2019)]. The…
Fromager and Lasorne [Electron. Struct. 6 025002 (2024)] have recently derived an in-principle exact Kohn-Sham density functional theory (KS-DFT) of electrons and nuclei, where the nuclear density and the (so-called conditional) electronic…
We show how a spin polarization can be generated through the photo-induced electron transfer of an achiral donor-acceptor complex following chiral light excitation. In particular, we illustrate the basic energetic and symmetry requirements…
Electron transfer (ET) at electrochemical interfaces is central to energy conversion and storage, yet its theoretical and computational modeling remain active research areas. This review elucidates key concepts and theories of ET kinetics,…