化学物理
Higher lying excited states beyond S1 and T1 are widely recognized in many photophysical systems, including thermally activated delayed fluorescence (TADF). However, their explicit and quantitative impact on photophysical observables such…
Standard harmonic-to-anharmonic thermodynamic integration (TI) is known to develop a near singularity in the integrand for solids exhibiting diffusive degrees of freedom, such as rotating functional groups or migrating defects. This…
High-throughput quantum-chemical calculations underpin modern molecular modelling, materials discovery, and machine-learning workflows, yet even semi-empirical methods become restrictive when many molecules must be evaluated. Here we report…
Quantum-state-controlled reactivity is a long-standing goal in the field of physical chemistry. In this work, we explore the vibrational-state-dependent behavior of the ion-molecule reaction between O2+ in distinct vibrational states and…
We study the strong-field interaction of a helical bi-chromatic pump with an anisotropic and inhomogeneous molecular system in the form of planar distribution of radially aligned molecular ensemble. This setting gives rise to macroscopic…
We investigate a diabatization procedure that localizes charges (in real space) and localizes spins (in spin space) for open-shell systems that exhibit charge transfer in the presence of spin-orbit coupling. The procedure is applied to a…
We present a generalized extension of the recently developed electron/hole-transfer Dynamically-weighted State-Averaged Constrained CASSCF (eDSC/hDSC) method to model charge transfer in the presence of spin-orbit coupling (SOC) for systems…
A data-driven computational method is introduced to extract chemical reaction mechanisms from time series chemical concentration data. It is realized through the use of dynamic symbolic regression in which a sparse analytical form for a…
Binding energies (BEs) of adsorbates on interstellar dust grains critically control adsorption, desorption, diffusion, and surface reactivity, and therefore strongly influence astrochemical models of star- and planet-forming regions. While…
Despite the great success Kohn-Sham density functional theory (KS-DFT) has achieved, the delocalization error remains a major challenge for commonly used density functional approximations (DFAs), resulting in systematic errors in ionization…
Coupled-cluster (CC) theory and Green's function many-body perturbation theory (MBPT) have long evolved as distinct yet complementary frameworks for describing electronic correlation. While CC methods employ exponential wavefunction…
We investigate ion pairing dynamics in electrolytes driven far from equilibrium using molecular simulations and nonequilibrium rate theory. Focusing on 0.5 M $\mathrm{LiPF_6}$ in water and acetonitrile under uniform electric fields, we…
Nuclear Magnetic Resonance (NMR) spectroscopy is fundamental for molecular structure elucidation, yet interpreting spectra at scale remains time-consuming and highly expertise-dependent. While recent spectrum-as-language modeling and…
Single crystals of C$_{60}$ saturated with molecular hydrogen and nitrogen were studied using the spectral-luminescent method of registration in the quantum counting mode at a low temperature of 20 K. Previously, it was found that the…
Transition states (TSs) are central to understanding and quantitatively predicting chemical reactivity and reaction mechanisms. Although traditional TS generation methods are computationally expensive, recent generative modeling approaches…
An in-principle exact working equation to compute electronic affinity and ionization Fukui functions is derived within the $N$-centered (Nc) ensemble extension of density functional theory (DFT). It circumvents the kernel derivative…
Quantum optimal control is central to designing spin manipulation pulses. Gradient-based pulse optimization can be facilitated by either accelerating gradient evaluation or enhancing the convergence rate. In this work, we accelerated…
The chiral-induced spin selectivity (CISS) effect demonstrates a strong coupling between electron spin and molecular chirality, enabling spin-controlled interactions between chiral molecules and magnetic surfaces. While CISS experiments…
In enzymatic recycling or biodegradation of semi-crystalline plastic waste, crystalline spherulites embedded into an amorphous matrix hinder and slow down depolymerisation. When the enzymatic depolymerisation temperature exceeds the glass…
We present a general computational protocol for the evaluation of extensive molecular response properties in complex environments within a polarizable quantum embedding framework. The approach extends multilevel density functional theory…