Imaging the Photochemistry of the Hydrogen-Bonded Heptazine-Water Complex with Femtosecond Time-Resolved Spectroscopy: A Computational StudyGraphitic carbon nitride (g-CN) has attracted vast interest as a promising inexpensive metal-free photocatalyst for water splitting with solar photons. The heptazine (Hz) molecule is the building…Sebastian V. Pios, Maxim F. Gelin, Wolfgang Domcke et al.·Nov 30, 2024SaveLearn
Basis set incompleteness errors in fixed-node diffusion Monte Carlo calculations on non-covalent interactionsBasis set incompleteness error (BSIE) is a common source of error in quantum chemistry (QC) calculations, but it has not been comprehensively studied in fixed-node Diffusion Monte Carlo (FN-DMC)…Kousuke Nakano, Benjamin X. Shi, Dario Alfè et al.·Nov 30, 2024SaveLearn
Neural Network Potential with Multi-Resolution Approach Enables Accurate Prediction of Reaction Free Energies in SolutionWe present design and implementation of a novel neural network potential (NNP) and its combination with an electrostatic embedding scheme, commonly used within the context of hybrid…Felix Pultar, Moritz Thuerlemann, Igor Gordiy et al.·Nov 29, 2024SaveLearn
OpenQDC: Open Quantum Data CommonsMachine Learning Interatomic Potentials (MLIPs) are a highly promising alternative to force-fields for molecular dynamics (MD) simulations, offering precise and rapid energy and force calculations.…Cristian Gabellini, Nikhil Shenoy, Stephan Thaler et al.·Nov 29, 2024SaveLearn
Hierarchical Framework for Retrosynthesis Prediction with Enhanced Reaction Center LocalizationRetrosynthesis is essential for designing synthetic pathways for complex molecules and can be revolutionized by AI to automate and accelerate chemical synthesis planning for drug discovery and…Seongeun Yun, Won Bo Lee·Nov 29, 2024SaveLearn
Low-Temperature Synthesis of Weakly Confined Carbyne inside Single-Walled Carbon NanotubesCarbyne, a one-dimensional (1D) carbon allotrope with alternating triple and single bonds, has the highest known mechanical strength but is unstable to bending, limiting synthesis to short linear…Bo-Wen Zhang, Xi-Yang Qiu, Yicheng Ma et al.·Nov 28, 2024SaveLearn
The Bigger the Better? Accurate Molecular Potential Energy Surfaces from Minimalist Neural NetworksAtomistic simulations are a powerful tool for studying the dynamics of molecules, proteins, and materials on wide time and length scales. Their reliability and predictiveness, however, depend…Silvan Käser, Debasish Koner, Markus Meuwly·Nov 27, 2024SaveLearn
SPARC-X-API: Versatile Python Interface for Real-space Density Functional Theory CalculationsDensity Functional Theory (DFT) is the de facto workhorse for large-scale electronic structure calculations in chemistry and materials science. While plane-wave DFT implementations remain the most…Tian Tian, Lucas R Timmerman, Shashikant Kumar et al.·Nov 27, 2024SaveLearn
Density-Functionalized QM/MM Delivers Chemical Accuracy For Solvated SystemsWe present a reformulation of QM/MM as a fully quantum mechanical theory of interacting subsystems, all treated at the level of density functional theory (DFT). For the MM subsystem, which lacks…Xin Chen, Jessica Martinez, Xuecheng Shao et al.·Nov 26, 2024SaveLearn
Nonequilibrium relaxation exponentially delays the onset of quantum diffusionPredicting the exact many-body quantum dynamics of polarons in materials with strong carrier-phonon interactions presents a fundamental challenge, often necessitating one to adopt approximations that…Srijan Bhattacharyya, Thomas Sayer, Andrés Montoya-Castillo·Nov 26, 2024SaveLearn
MOLPIPx: an end-to-end differentiable package for permutationally invariant polynomials in Python and RustIn this work, we present MOLPIPx, a versatile library designed to seamlessly integrate Permutationally Invariant Polynomials (PIPs) with modern machine learning frameworks, enabling the efficient…Manuel S. Drehwald, Asma Jamali, Rodrigo A. Vargas-Hernández·Nov 26, 2024SaveLearn
Broadband Cavity-Enhanced Absorption Spectroscopy (BBCEAS) Coupled with an Interferometer for On-Band and Off-Band Detection of GlyoxalGlyoxal CHOCHO is a trace gas in the atmosphere, often used as an indicator of biogenic emissions. It is frequently compared to formaldehyde concentrations, which serve as indicators of anthropogenic…Callum E. Flowerday, Ryan Thalman, Matthew C. Asplund et al.·Nov 25, 2024SaveLearn
Review of the foundations of time-dependent density-functional theory (TDDFT)Time-dependent density-functional theory (TDDFT) is deemed to be a formally rigorous way of dealing with the time-evolution of a many-electron system at the level of electron densities rather than…Jochen Schirmer·Nov 25, 2024SaveLearn
Accurate and Efficient Prediction of Double Excitation Energies Using the Particle-Particle Random Phase ApproximationDouble excitations are crucial to understanding numerous chemical, physical, and biological processes, but accurately predicting them remains a challenge. In this work, we explore the…Jincheng Yu, Jiachen Li, Tianyu Zhu et al.·Nov 25, 2024SaveLearn
Variational functional theory for coulombic correlations in the electric double layerA classical coulombic correlation functional in one-loop (1L) and local-density-approximation (LDA) is derived for electrolyte solutions, starting from a first-principles many-body partition…Nils Bruch, Tobias Binninger, Jun Huang et al.·Nov 25, 2024SaveLearn
Observation of a core-excited dipole-bound state 1 eV above the electron detachment threshold in cryogenically cooled acetylacetonateDipole-bound states in anions exist when a polar neutral core binds an electron in a diffuse orbital through charge--dipole interaction. Electronically excited polar neutral cores can also bind an…Rafael A Jara-Toro, Martín Taccone, Jordan Dezalay et al.·Nov 25, 2024SaveLearn
A constant potential reactor framework for electrochemical reaction simulationsUnderstanding the evolution of electrified solid-liquid interfaces during electrochemical reactions is crucial. However, capturing the dynamic behavior of the interfaces with high temporal resolution…Letian Chen, Yun Tian, Xu Hu et al.·Nov 25, 2024SaveLearn
High temperature melting of dense molecular hydrogen from machine-learning interatomic potentials trained on quantum Monte CarloWe present results and discuss methods for computing the melting temperature of dense molecular hydrogen using a machine learned model trained on quantum Monte Carlo data. In this newly trained…Shubhang Goswami, Scott Jensen, Yubo Yang et al.·Nov 23, 2024SaveLearn
Constant-Potential Machine Learning Molecular Dynamics Simulations Reveal Potential-Regulated Cu Cluster Formation on MoS2Electrochemical processes play a crucial role in energy storage and conversion systems, yet their computational modeling remains a significant challenge. Accurately incorporating the effects of…Jingwen Zhou, Yunsong Fu, Ling Liu et al.·Nov 22, 2024SaveLearn
Quantum mechanical deconstruction of vibrational energy transfer rate and pathways modified by collective vibrational strong couplingRecent experiments have demonstrated that vibrational strong coupling (VSC) between molecular vibrations and the optical cavity field can modify vibrational energy transfer (VET) processes in…Qi Yu, Dong H. Zhang, Joel M. Bowman·Nov 22, 2024SaveLearn
Singlet Fission in Carotenoid Dimers -- The Role of the Exchange and Dipolar InteractionsA theory of singlet fission in carotenoid dimers is presented which aims to explain the mechanism behind the creation of two uncorrelated triplets. Following the initial photoexcitation of a…Alexandru G. Ichert, William Barford·Nov 21, 2024SaveLearn
Simulating Nonadiabatic Dynamics in Benzophenone: Tracing Internal Conversion Through Photoelectron SpectraBenzophenone serves as a prototype chromophore for studying the photochemistry of aromatic ketones, with applications ranging from biochemistry to organic light-emitting diodes. In particular, its…Lorenzo Restaino, Thomas Schnappinger, Markus Kowalewski·Nov 21, 2024SaveLearn
On the applicability of CCSD(T) for dispersion interactions in large conjugated systemsIn light of the recent discrepancies reported between fixed node diffusion Monte Carlo and local natural orbital coupled cluster with single, double and perturbative triples (CCSD(T)) methodologies…S. Lambie, D. Kats, D. Usyvat et al.·Nov 21, 2024SaveLearn
Lithium-ion battery modelling for nonisothermal conditionsA nonequilibrium thermodynamic model is presented for the nonisothermal lithium-ion battery cell. Coupling coefficients, all significant for transport of heat, mass, charge and chemical reaction,…Felix Schloms, Øystein Gullbrekken, Signe Kjelstrup·Nov 21, 2024SaveLearn
A Phase-Space Electronic Hamiltonian for Molecules in a Static Magnetic Field II: Quantum Chemistry Calculations with Gauge Invariant Atomic OrbitalsIn a companion paper, we have developed a phase-space electronic structure theory of molecules in magnetic fields, whereby the electronic energy levels arise from diagonalizing a phase-space…Mansi Bhati, Zhen Tao, Xuezhi Bian et al.·Nov 21, 2024SaveLearn