化学物理
Liquid-liquid equilibria phase diagrams have been determined for the systems: 2-methoxyphenol + n-decane, or + n-dodecane, or + n-tetradecane or + n-hexadecane and for 2-ethoxyphenol + n-octane, or + n-dodecane, or + n-tetradecane, or +…
Thermodynamics, introduced over two centuries ago, remains foundational to our understanding of physical, chemical, biological, and engineering systems. Its principles are traditionally grounded in the statistical mechanics framework, which…
Dispersion of collective excitations in fluid Hydrogen along the isothermal line T=2500~K, including the region of molecular-to-atomis fluid transition, is studied by ab initio molecular dynamics (AIMD) simulations. The obtained density…
We study the photoinduced chemical dynamics of cyclobutanone upon excitation at 200 nm to the 3s Rydberg state using MeV ultrafast electron diffraction (UED). We observe both the elastic scattering signal, which contains information about…
Graph Neural Network (GNN) potentials relying on chemical locality offer near-quantum mechanical accuracy at significantly reduced computational costs. Message-passing GNNs model interactions beyond their immediate neighborhood by…
Molecular structures with multiple donor, bridge, or acceptor units can display quantum interference effects that influence electron and energy transfer (ET and EnT) rates. Recent experiments found a 4- to 5-fold increase in ET rates for…
Gem-dicarbonyls of transition metals supported on metal (oxide) surfaces are common intermediates in heterogeneous catalysis. While infrared (IR) spectroscopy is a standard tool for detecting these species on applied catalysts, the…
A key challenge in ultrafast science has been to directly track the coupled motions of electrons and nuclei in real-space and real-time. This study presents a significant step towards this goal by demonstrating the feasibility of…
Circularly-polarized (CP) vibrations are the nuclear-motion analog of CP light, emerging in molecules with non-Abelian point-group symmetry that support orthogonal and degenerate vibrational normal modes. Here, we explore the optical…
In the present work, we present a hybrid quantum-classical workflow aimed at improving the accuracy of alchemical free energy (AFE) predictions by incorporating configuration interaction (CI) simulations using the book-ending correction…
To reduce the complexity of infrared spectroscopy hardware while maintaining performance, a data informed, task-specific, spectral collection approach termed Sparse Infrared Spectroscopy (SIRS) is developed. Using a numerically based…
Addressing both dynamic and static correlation accurately is a primary goal in electronic structure theory. Non-orthogonal configuration interaction (NOCI) is a versatile tool for treating static correlation, offering chemical insights by…
Accounting for dispersion interactions is essential in approximate density functional theory (DFT). Often, a correction potential based on the London formula is added, which is damped at short distances to avoid divergence and double…
Reliable description of bond breaking remains a major challenge for quantum chemistry due to the multireferential character of the electronic structure in dissociating species. Multireferential methods in particular suffer from large…
Traditional atomistic machine learning (ML) models serve as surrogates for quantum mechanical (QM) properties, predicting quantities such as dipole moments and polarizabilities, directly from compositions and geometries of atomic…
Thermodynamic models and, in particular, SAFT-type equations are vital in characterizing complex systems. This paper presents a framework for sampling parameter distributions in PC-SAFT and SAFT-VR Mie equations of state to understand…
Coarse-grained (CG) molecular dynamics simulations extend the length and time scale of atomistic simulations by replacing groups of correlated atoms with CG beads. Machine-learned coarse-graining (MLCG) has recently emerged as a promising…
Nanoalloys offer a unique opportunity to tailor chemical properties through changes in composition, shape, and size. However, this flexibility introduces complexity that challenges both experimental and conventional theoretical methods. In…
We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard X-ray scattering. Time-resolved X-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the…
Given the power of large language and large vision models, it is of profound and fundamental interest to ask if a foundational model based on data and parameter scaling laws and pre-training strategies is possible for learned simulations of…