化学物理
The formation of H$^{3+}$ from ethane, propane, and butane dications was investigated with time-dependent density-functional theory (TDDFT) simulations. This approach offers the benefit of simultaneously addressing nuclear and electronic…
We propose a non-iterative, post hoc correction to the unitary coupled cluster theory with single, double, and triple excitations (UCCSDT) ansatz, which considers the leading-order effects of neglected quadruple excitations. We present two…
Silicon is the most important semiconductor electrode with applications in photoelectrochemistry and sensor technology. Yet its electrochemistry exhibits many poorly understood phenomena, including oscillations during the anodic dissolution…
We propose Ehrenfest Dynamics with Spontaneous Localization (SLED), a decoherence-corrected extension of Ehrenfest dynamics based on the Gisin-Percival quantum-state diffusion (QSD) equation. In SLED, the electronic wavefunction evolves…
The selection of suitable ionic liquids (ILs) is critical for CO2 capture and electrocatalytic conversion into valuable chemical products. The screening process can be enhanced with theoretical simulations that reveal the…
Conventional methods for modeling thermocatalytic systems are typically based on the Kohn-Sham density functional theory (KS-DFT), neglecting the inhomogeneous distributions of gas molecules in the reactive environment. However, industrial…
The on-demand manipulation of triplet states in closed-shell single molecules is still out of reach due to a lack of information about the energy of those triplet states. Yet, the access to triplet states would open up a route towards an…
Fourier Transform (FT) has been a mainstay of analytical 13C and 15N NMR. On the other hand it has been shown that Steady State Free Precession (SSFP) experiments which depart from this scheme can, under certain conditions, endow 13C and…
We extend the existing framework of macroscopic HHG to combine it with high-accuracy ab initio calculations for molecules as microscopic input. This approach is applied to HHG spectra exhibiting Mollow sidebands, for open shell molecules…
Organic reaction, the foundation of modern chemical industry, is crucial for new material development and drug discovery. However, deciphering reaction mechanisms and modeling multi-molecular relationships remain formidable challenges due…
We present a mixed basis-set approach to obtain optical absorption spectra within a generalized Kohn-Sham time-dependent density functional theory framework. All occupied valence molecular orbitals (MOs) are expanded in a plane-wave (PW)…
Machine learning (ML) has emerged as a promising tool for simulating quantum dissipative dynamics. However, existing methods often struggle to enforce key physical constraints, such as trace conservation, when modeling reduced density…
Quantum Selected Configuration Interaction (QSCI) methods (also known as Sample-based Quantum Diagonalization, SQD) have emerged as promising near-term approaches to solving the electronic Schr{\"o}dinger equation with quantum computers. In…
Understanding the performance of electrochemical energy storage systems requires probing the electrochemical properties at each layer and interface during cell operation. While traditional onboard and operando methods can measure impedance,…
Quantum computing presents a promising avenue for solving complex problems, particularly in quantum chemistry, where it could accelerate the computation of molecular properties and excited states. This work focuses on hybrid…
The field of computational chemistry is increasingly leveraging machine learning (ML) potentials to predict molecular properties with high accuracy and efficiency, providing a viable alternative to traditional quantum mechanical (QM)…
Unlike with the energy, which is a scalar property, machine learning (ML) predictions of vector or tensor properties poses the additional challenge of achieving proper invariance (covariance) with respect to molecular rotation. If the…
The hydrogen evolution reaction (HER) in alkaline media suffers from sluggish kinetics but the origin of the pH-dependent activity remains debated. This study investigates the role of hydroxide ions (OH) in enhancing the alkaline HER at…
The connect-fill-run workflow paradigm, widely adopted in mature software engineering, accelerates collaborative development. However, computational chemistry, computational materials science, and computational biology face persistent…
In this work, we describe a new algorithm, O1NumHess, to calculate the Hessian of a molecular system by finite differentiation of gradients calculated at displaced geometries. Different from the conventional seminumerical Hessian algorithm,…