Ultrafast Photochemistry and Electron Diffraction for Cyclobutanone in the S2 State: Surface Hopping with Time-Dependent Density Functional TheoryWe simulate the photodynamics of gas-phase cyclobutanone excited to the S2 state using fewest switches surface hopping (FSSH) dynamics powered by time-dependent density functional theory (TDDFT).…Ericka Roy Miller, Sean J. Hoehn, Abhijith Kumar et al.·Feb 15, 2024SaveLearn
ChemReasoner: Heuristic Search over a Large Language Model's Knowledge Space using Quantum-Chemical FeedbackThe discovery of new catalysts is essential for the design of new and more efficient chemical processes in order to transition to a sustainable future. We introduce an AI-guided computational…Henry W. Sprueill, Carl Edwards, Khushbu Agarwal et al.·Feb 15, 2024SaveLearn
Using a multistate Mapping Approach to Surface Hopping to predict the Ultrafast Electron Diffraction signal of gas-phase cyclobutanoneUsing the recently developed multistate mapping approach to surface hopping (multistate MASH) method combined with SA(3)-CASSCF(12,12)/aug-cc-pVDZ electronic structure calculations, the gas-phase…Lewis Hutton, Andres Moreno Carrascosa, Andrew W. Prentice et al.·Feb 15, 2024SaveLearn
OH-Formation Following Vibrationally Induced Reaction Dynamics of H2COOThe reaction dynamics of H2COO to form linear HCOOH and dioxirane as first steps for OH-elimination is quantitatively investigated. Using a machine learned potential energy surface at the…Kaisheng Song, Meenu Upadhyay, Markus Meuwly·Feb 15, 2024SaveLearn
Prediction Through Quantum Dynamics Simulations: Photo-excited CyclobutanoneQuantum dynamics simulations are becoming a standard tool for simulating photo-excited molecular systems involving a manifold of coupled states, known as non-adiabatic dynamics. While these…Olivia Bennett, Antonia Freibert, K. Eryn Spinlove et al.·Feb 15, 2024SaveLearn
Prediction Challenge: Simulating Rydberg Photoexcited Cyclobutanone with Surface Hopping Dynamics based on Different Electronic Structure MethodsThis research examines the nonadiabatic dynamics of cyclobutanone after excitation into the n-3s Rydberg S2 state. It stems from our contribution to the Special Topic of the Journal of Chemical…Saikat Mukherjee, Rafael S. Mattos, Josene M. Toldo et al.·Feb 15, 2024SaveLearn
Ultrafast photochemistry and electron-diffraction spectra in n->(3s) Rydberg excited cyclobutanone resolved at the multireference perturbative levelWe study the ultrafast time evolution of cyclobutanone excited to singlet n-->Rydberg state through XMS-CASPT2 nonadiabatic surface-hopping simulations. These dynamics predict relaxation to…V. K. Jaiswal, F. Montorsi, F. Aleotti et al.·Feb 15, 2024SaveLearn
The Photochemistry of Rydberg Excited Cyclobutanone: Photoinduced Processes and Ground State DynamicsOwing to ring-strain, cyclic ketones exhibit complex excited-state dynamics with multiple competing photochemical channels active on the ultrafast timescale. While the excited-state dynamics of…Julien Eng, Conor Rankine, Thomas Penfold·Feb 14, 2024SaveLearn
The photodissociation dynamics and ultrafast electron diffraction image of cyclobutanone from the surface hopping dynamics simulationThe comprehension of nonadiabatic dynamics in polyatomic systems relies heavily on the simultaneous advancements in theoretical and experimental domains. The gas-phase electron diffraction (GUED)…Jiawei Peng, Hong Liu, Zhenggang Lan·Feb 14, 2024SaveLearn
Bayesian Multistate Bennett Acceptance Ratio MethodsThe multistate Bennett acceptance ratio (MBAR) method is a prevalent approach for computing free energies of thermodynamic states. In this work, we introduce BayesMBAR, a Bayesian generalization of…Xinqiang Ding·Feb 14, 2024SaveLearn
Spin-coupled molecular orbitals: chemical intuition meets quantum chemistryMolecular orbital theory is powerful both as a conceptual tool for understanding chemical bonding, and as a theoretical framework for ab initio quantum chemistry. Despite its undoubted success, MO…Daniel Marti-Dafcik, Nicholas Lee, Hugh G. A. Burton et al.·Feb 13, 2024SaveLearn
An assessment of frozen natural orbitals and band gaps using equation of motion coupled cluster theory: a case study on polyacene and trans-polyacetyleneFrozen natural orbitals (FNOs) are used to augment IP/EA-EOM-CCSD calculations targeting the band gap of trans-polyacetylene and polyacene. We show the resulting electron affinities (EAs), ionization…Zachary W. Windom, AV Lam, Ajith Perera et al.·Feb 13, 2024SaveLearn
Zero Shot Molecular Generation via Similarity KernelsGenerative modelling aims to accelerate the discovery of novel chemicals by directly proposing structures with desirable properties. Recently, score-based, or diffusion, generative models have…Rokas Elijošius, Fabian Zills, Ilyes Batatia et al.·Feb 13, 2024SaveLearn
Unveiling interatomic distances influencing the reaction coordinates in alanine dipeptide isomerization: An explainable deep learning approachThe present work shows that the free energy landscape associated with alanine dipeptide isomerization can be effectively represented by specific interatomic distances without explicit reference to…Kazushi Okada, Takuma Kikutsuji, Kei-ichi Okazaki et al.·Feb 13, 2024SaveLearn
VAMPyR -- A High-Level Python Library for Mathematical Operations in a Multiwavelets RepresentationWavelets and Multiwavelets have lately been adopted in Quantum Chemistry to overcome challenges presented by the two main families of basis sets: Gaussian atomic orbitals and plane waves. In addition…Magnar Bjørgve, Christian Tantardini, Stig Rune Jensen et al.·Feb 13, 2024SaveLearn
Structural Descriptors and Information Extraction from X-ray Emission Spectra: Aqueous Sulfuric AcidMachine learning can reveal new insights into X-ray spectroscopy of liquids when the local atomistic environment is presented to the model in a suitable way. Many unique structural descriptor…E. A. Eronen, A. Vladyka, Ch. J. Sahle et al.·Feb 13, 2024SaveLearn
Mixing due to Solution-switch Limits the Performance of Electro-sorption for DesalinationElectro-sorption (ES) is a research frontier in electrochemical separation, with proven potential applications in desalination, wastewater treatment, and selective resource extraction. However, due…Weifan Liu, Longqian Xu, Zezhou Yang et al.·Feb 13, 2024SaveLearn
Anisotropic molecular photoemission dynamics: Interpreting and accounting for the nuclear motionWe investigate how vibration affects molecular photoemission dynamics, through simulations on two-dimension asymmetric model molecules including the electronic and nuclear motions in a fully…Antoine Desrier, Morgan Berkane, Camille Lévêque et al.·Feb 12, 2024SaveLearn
Measuring friction from simulations of folded graphene sheetsWe run molecular dynamics simulations of folded graphene sheets and present a procedure to measure the sliding friction in these systems based on the rate of decay of a damped-harmonic oscillator.…Charlie M. Rawlins, Gareth A. Tribello·Feb 12, 2024SaveLearn
Charge emissions from Electrosprays in vacuum: mixtures of formamide with methylammonium formateThe charge/mass distribution f(q/m) of nanodrops and ions electrosprayed in vacuum from mixtures of formamide (FM) and methylammonium formate (MAF) is studied by time of flight mass spectrometry at…David Garoz, Juan Fernández de la Mora·Feb 11, 2024SaveLearn
Quantum Quality with Classical Cost: Ab Initio Nonadiabatic Dynamics Simulations using the Mapping Approach to Surface HoppingNonadiabatic dynamics methods are an essential tool for investigating photochemical processes. In the context of employing first principles electronic structure techniques, such simulations can be…Jonathan R. Mannouch, Aaron Kelly·Feb 11, 2024SaveLearn
Accelerating molecular vibrational spectra simulations with a physically informed deep learning modelIn recent years, machine learning (ML) surrogate models have emerged as an indispensable tool to accelerate simulations of physical and chemical processes. However, there is still a lack of ML models…Yuzhuo Chen, Sebastian V. Pios, Maxim F. Gelin et al.·Feb 10, 2024SaveLearn
Binding Selectivity Analysis from Alchemical Receptor Hopping and Swapping Free Energy CalculationsWe present receptor hopping and receptor swapping free energy estimation protocols based on the Alchemical Transfer Method (ATM) to model the binding selectivity of a set of ligands to two arbitrary…Solmaz Azimi, Emilio Gallicchio·Feb 10, 2024SaveLearn
Benchmarking ionization potentials from pCCD tailored coupled cluster modelsThe ionization potential (IP) is an important parameter providing essential insights into the reactivity of chemical systems. IPs are also crucial for designing, optimizing, and understanding the…Marta Gałyńska, Katharina Boguslawski·Feb 9, 2024SaveLearn
Radiationless decay spectrum of O 1s double core holes in liquid waterWe present a combined experimental and theoretical investigation of the radiationless decay spectrum of an O 1s double core hole in liquid water. Our experiments were carried out using liquid-jet…Florian Trinter, Ludger Inhester, Ralph Püttner et al.·Feb 9, 2024SaveLearn