化学物理
Using GPU-accelerated state-vector emulation, we propose to embed a quantum computing ansatz into density-functional theory via density-based basis-set corrections (DBBSC) to obtain quantitative quantum-chemistry results on molecules that…
Transient absorption spectroscopy (TAS) is among the most common ultrafast photochemical experiments, but its interpretation remains challenging. In this work, we present an efficient and robust method for simulating TAS signals from first…
Computer simulation has long been an essential partner of ultrafast experiments, allowing the assignment of microscopic mechanistic detail to low-dimensional spectroscopic data. However, the ability of theory to make a priori predictions of…
Controlling structural transitions between molecular configurations is crucial for advancing functional molecular electronics. While reversible switching of bistable two-state molecules has been achieved, creating molecular systems that can…
Coarse-graining is a molecular modeling technique in which an atomistic system is represented in a simplified fashion that retains the most significant system features that contribute to a target output, while removing the degrees of…
We present an efficient implementation of multireference algebraic diagrammatic construction theory (MR-ADC) for simulating core-ionized states and X-ray photoelectron spectra (XPS). Taking advantage of spin adaptation, automatic code…
The concept of Dyall zeroth-order Hamiltonian [Dyall, K. G. J. Chem. Phys., 102, 4909-4918 (1995)] has been instrumental in the development of intruder- and parameter-free multireference perturbation theories for the efficient treatment of…
Using normalizing flows and reweighting, Boltzmann Generators enable equilibrium sampling from a Boltzmann distribution, defined by an energy function and thermodynamic state. In this work, we introduce Thermodynamic Interpolation (TI),…
Fluid-solid interfacial free energy (IFE) is a fundamental parameter influencing wetting behaviors, which play a crucial role across a broad range of industrial applications. Obtaining reliable data for fluid-solid IFE remains challenging…
Experiments show that light-matter strong coupling affects chemical properties, though the underlying mechanism remains unclear. We present an ab initio quantum electrodynamics coupled cluster method for the collective strong coupling…
Multi-criteria decision making (MCDM) is necessary for choosing one from the available alternatives (or from the obtained Pareto-optimal solutions for multi-objective optimization), where the performance of each alternative is quantified…
Highly excited C$_2{}^{-}$ ions prominently feature electron detachment at a mean decay time near 3 milliseconds with hitherto unexplained origin. Considering various sources of unimolecular decay, we attribute the signal to the electronic…
On the millisecond to second time scale, stored beams of diatomic carbon anions C$_2{}^-$ from a sputter ion source feature unimolecular decay of yet unexplained origin by electron emission and fragmentation. To account for the magnitude…
Time-dependent Hartree-Fock (TDHF) is one of the fundamental post-Hartree-Fock (HF) methods to describe excited states. In its Tamm-Dancoff form, equivalent to Configuration Interaction Singles, it is still widely used and particularly…
Electrolyte solutions play critical role in a vast range of important applications, yet an accurate and scalable method of predicting their properties without fitting to experiment has remained out of reach, despite over a century of…
As crucial additives and intermediate, alcohols, ethers, and aldehydes play a significant role in the combustion process. However, the chemistry of NOXhydrocarbon interactions and the rate rules governing these interactions remain largely…
Minimum energy conical intersections can be used to rationalize photochemical processes. In this Letter, we examine an algorithm to locate these structures that does not require the evaluation of nonadiabatic coupling vectors, showing that…
Compared to ground state electronic structure optimizations, accurate simulations of molecular real-time electron dynamics are usually much more difficult to perform. To simulate electron dynamics, the time-dependent density matrix…
The effect of replacing individual contributions to an empirical energy function are assessed for halogenated benzenes (X-Bz, X = H, F, Cl, Br) and chlorinated phenols (Cl-PhOH). Introducing electrostatic models based on distributed charges…
The exact quantum dynamics of lattice models can be computationally intensive, especially when aiming for large system sizes and extended simulation times necessary to converge transport coefficients. By leveraging finite memory times to…