化学物理
Predicting the ground-state 3D molecular conformations from 2D molecular graphs is critical in computational chemistry due to its profound impact on molecular properties. Deep learning (DL) approaches have recently emerged as promising…
Electrolytes mediate interactions between the cathode and anode and determine performance characteristics of batteries. Mixtures of multiple solvents are often used in electrolytes to achieve desired properties, such as viscosity,…
Rechargeable batteries that incorporate shaped three-dimensional electrodes have been shown to have increased power and energy densities for a given footprint area when compared to a conventional geometry, i.e., a planar cathode and anode…
The exchange-only virial relation due to Levy and Perdew is revisited. Invoking the adiabatic connection, we introduce the exchange energy in terms of the right-derivative of the universal density functional w.r.t. the coupling strength…
The success of language models, especially transformer-based architectures, has trickled into other domains giving rise to "scientific language models" that operate on small molecules, proteins or polymers. In chemistry, language models…
The Hohenberg-Kohn theorem of density-functional theory (DFT) is broadly considered the conceptual basis for a full characterization of an electronic system in its ground state by just the one-body particle density. In this Part~II of a…
The Hohenberg-Kohn theorem of density-functional theory (DFT) is broadly considered the conceptual basis for a full characterization of an electronic system in its ground state by just the one-body particle density. Part I of this review…
Density-functional theory requires an extra variable besides the electron density in order to properly incorporate magnetic-field effects. In a time-dependent setting, the gauge-invariant, total current density takes that role. A peculiar…
The presence of two chlorine atoms in 1,2-dichloroethene allows for isomerisation around the double bond. This isomerisation can lead to rich photochemistry. We present a time-resolved pump-probe photoelectron spectroscopy measurement on…
Modern machine learning (ML) models of chemical and materials systems with billions of parameters require vast training datasets and considerable computational efforts. Lightweight kernel or decision tree based methods, however, can be…
Excited state proton transfer is an ubiquitous phenomenon in biology and chemistry, spanning from the ultrafast reactions of photo-bases and acids to light-driven, enzymatic catalysis and photosynthesis. However, the simulation of such…
A circularly polarized laser pulse can induce persistent intra-molecular currents by either exciting or ionizing molecules. These two cases are identified as electron currents and hole currents, respectively, and up to now they have been…
The accelerated demand for electrochemical energy storage urges the need for new, sustainable, stable and lightweight materials able to store high energy densities rapidly and efficiently. Development of these functional materials requires…
A brush structure is an interesting object for future applications in medical and electronic devices. Usual substrate for the brushes is silicon wafer with linker molecules. In present study an ion beam treatment of polymer was used for…
Over the last decades, theoretical photochemistry has produced multiple techniques to simulate the nonadiabatic dynamics of molecules. Surprisingly, much less effort has been devoted to adequately describing the first step of a…
We extend the DeePMD neural network architecture to predict electronic structure properties necessary to perform non-adiabatic dynamics simulations. While learning the excited state energies and forces follows a straightforward extension of…
Transition states (TSs) are transient structures that are key in understanding reaction mechanisms and designing catalysts but challenging to be captured in experiments. Alternatively, many optimization algorithms have been developed to…
Transition state theory is a standard framework for predicting the rate of a chemical reaction. Although the transition state theory has been successfully applied to numerous chemical reaction analyses, many experimental and theoretical…
Inspired by recent visible pump - infrared probe spectra reported for molecular catalysts adsorbed to quantum dots, we introduce a theory of non-equilibrium vibronic Fano resonances arising from the interference of quantum dot excited-state…
The racemization of amino acids constitutes one of the most elemental and critical reactions, holding primitive significance for understanding the life's origin and maintenance. Nevertheless, its mechanism at the atomic level has been…