A Phase-Space Electronic Hamiltonian for Molecules in a Static Magnetic Field I: Conservation of Total Pseudomomentum and Angular MomentumWe develop a phase-space electronic structure theory of molecules in magnetic fields. For a system of electrons in a magnetic field with vector potential A(r), the usual…Mansi Bhati, Zhen Tao, Xuezhi Bian et al.·Nov 21, 2024SaveLearn
Beyond Dielectrics: Interfacial Water Polarization Governs Graphene-Based Electrochemical InterfacesWater molecules are traditionally regarded as passive dielectric media in electrochemical systems. In this work, we challenge this conventional perspective using molecular dynamics simulations and…Peiyao Wang, Gengping Jiang, Yuan Yan et al.·Nov 20, 2024SaveLearn
The vDZP Basis Set Is Effective For Many Density FunctionalsIn recent years, "composite" density-functional-theory-based methods comprising specially optimized combinations of functionals, basis sets, and empirical corrections have become widely used owing to…Corin C. Wagen, Jonathon E. Vandezande·Nov 20, 2024SaveLearn
Anomalous propagators and the particle-particle channel: Bethe-Salpeter equationThe Bethe-Salpeter equation has been extensively employed to compute the two-body electron-hole propagator and its poles which correspond to the neutral excitation energies of the system. Through a…Antoine Marie, Pina Romaniello, Xavier Blase et al.·Nov 20, 2024SaveLearn
When Theory Meets Experiment: What Does it Take to Accurately Predict 1H NMR Dipolar Relaxation Rates in Neat Liquid Water from Theory?In this contribution, we compute the 1H nuclear magnetic resonance (NMR) relaxation rate of liquid water at ambient conditions. We are using structural and dynamical information from Coupled…Dietmar Paschek, Johanna Busch, Angel Mary Chiramel Tony et al.·Nov 19, 2024SaveLearn
A polarizable CASSCF/MM approach using the interface between OpenMMPol library and CFourWe present a polarizable embedding quantum mechanics/molecular mechanics (QM/MM) framework for ground- and excited-state Complete Active Space Self-Consistent Field (CASSCF) calculations on molecules…Tommaso Nottoli, Mattia Bondanza, Filippo Lipparini et al.·Nov 19, 2024SaveLearn
Balancing property optimization and constraint satisfaction for constrained multi-property molecular optimizationMolecular optimization, which aims to discover improved molecules from a vast chemical search space, is a critical step in chemical development. Various artificial intelligence technologies have…Xin Xia, Yajie Zhang, Xiangxiang Zeng et al.·Nov 19, 2024SaveLearn
Post-CCSD(T) corrections in the S66 noncovalent interactions benchmarkFor noncovalent interactions, it is generally assumed that CCSD(T) is nearly the exact solution within the 1-particle basis set. For the S66 noncovalent interactions benchmark, we present for the…Emmanouil Semidalas, A. Daniel Boese, Jan M. L. Martin·Nov 18, 2024SaveLearn
MixPI: Mixed-Time Slicing Path Integral Software for Quantized Molecular Dynamics SimulationsPath Integral Molecular Dynamics (PIMD) is a well established simulation technique to compute exact equilibrium properties for a quantum system using classical trajectories in an extended phase…Britta A. Johnson, Siyu Bu, Christopher J. Mundy et al.·Nov 18, 2024SaveLearn
Extension of the Active-Orbital-Based and Adaptive CC(P;Q) Approaches to Excited Electronic States: Application to Potential Cuts of WaterWe report the first study using active-orbital-based and adaptive CC(P;Q) approaches to describe excited electronic states. These CC(P;Q) methodologies are applied, alongside their completely…Karthik Gururangan, Jun Shen, Piotr Piecuch·Nov 18, 2024SaveLearn
Electron Phase Detection in Single Molecules by InterferometryInterferometry has underpinned a century of discoveries, ranging from the disproval of the ether theory to the detection of gravitational waves, offering insights into wave dynamics with unrivalled…Zhixin Chen, Jie-Ren Deng, Mengyun Wang et al.·Nov 18, 2024SaveLearn
Depth-resolved measurement of solvation entropy, interfacial transport and charge-transfer kinetics of practical lithium-ion batteriesUnderstanding the performance of electrochemical energy storage systems requires probing the electrochemical properties at each layer and interface during cell operation. While traditional onboard…Divya Chalise, Sean D. Lubner, Sumanjeet Kaur et al.·Nov 17, 2024SaveLearn
Quantum Chemical and Trajectory Surface Hopping Molecular Dynamics Study of Iodine-based BODIPY PhotosensitizerA computational study of I-BODIPY (2-ethyl-4,4-difluoro-6,7-diiodo-1,3-dimethyl-4-bora-3a,4a-diaza-s-indacene) was conducted to investigate its photophysical properties as a potential triplet…Mirza Wasif Baig, Marek Pederzoli, Mojmír Kývala et al.·Nov 16, 2024SaveLearn
Simulating Ionized States in Realistic Chemical Environments With Algebraic Diagrammatic Construction Theory and Polarizable EmbeddingTheoretical simulations of electron detachment processes are vital for understanding chemical redox reactions, semiconductor and electrochemical properties, and high-energy radiation damage. However,…James D. Serna, Alexander Yu. Sokolov·Nov 15, 2024SaveLearn
Linear Response pCCD-Based Methods: LR-pCCD and LR-pCCD+S Approaches for the Efficient and Reliable Modeling of Excited state PropertiesIn this work, we derive working equations for the Linear Response pair Coupled Cluster Doubles (LR-pCCD) ansatz and its extension to singles (S), LR-pCCD+S. These methods allow us to compute…Somayeh Ahmadkhani, Katharina Boguslawsk, Paweł Tecmer·Nov 15, 2024SaveLearn
Self-learning path integral hybrid Monte Carlo with mixed ab initio and machine learning potentials for modeling nuclear quantum effects in waterThe introduction of machine learned potentials (MLPs) has greatly expanded the space available for studying Nuclear Quantum Effects computationally with ab initio path integral (PI) accuracy, with…Bo Thomsen, Yuki Nagai, Keita Kobayashi et al.·Nov 15, 2024SaveLearn
Thermodynamic Interpolation: A generative approach to molecular thermodynamics and kineticsUsing normalizing flows and reweighting, Boltzmann Generators enable equilibrium sampling from a Boltzmann distribution, defined by an energy function and thermodynamic state. In this work, we…Selma Moqvist, Weilong Chen, Mathias Schreiner et al.·Nov 15, 2024SaveLearn
Estimating Fluid-solid Interfacial Free Energies for Wettabilities: A Review of Molecular Simulation MethodsFluid-solid interfacial free energy (IFE) is a fundamental parameter influencing wetting behaviors, which play a crucial role across a broad range of industrial applications. Obtaining reliable data…Yafan Yang, Arun Kumar Narayanan Nair, Shuyu Sun et al.·Nov 15, 2024SaveLearn
NEP-MB-pol: A unified machine-learned framework for fast and accurate prediction of water's thermodynamic and transport propertiesWater's unique hydrogen-bonding network and anomalous properties pose significant challenges for accurately modeling its structural, thermodynamic, and transport behavior across varied conditions.…Ke Xu, Ting Liang, Nan Xu et al.·Nov 14, 2024SaveLearn
Chemical bonding in three-membered ring systemsThe formation of the four three-ring systems c-(CH2)3-k(SiH2)k, (k=0: cyclopropane, k=1: silirane, k=2: disilirane, k=3: cyclotrisilane) by addition of methylene and silylene to…Nina Strasser, Alexander F. Sax·Nov 14, 2024SaveLearn
On the H-atom abstractions from C1-C4 alcohols, aldehydes, and ethers by NO2: ab initio and comprehensive kinetic modelingAs crucial additives and intermediate, alcohols, ethers, and aldehydes play a significant role in the combustion process. However, the chemistry of NOXhydrocarbon interactions and the rate rules…Hongqing Wu^, Ruoyue Tang^, Yuxin Dong et al.·Nov 14, 2024SaveLearn
Machine Learning-Based Enhancements of Empirical Energy Functions: Structure, Dynamics and Spectroscopy of Modified BenzenesThe effect of replacing individual contributions to an empirical energy function are assessed for halogenated benzenes (X-Bz, X = H, F, Cl, Br) and chlorinated phenols (Cl-PhOH). Introducing…Kham Lek Chaton, Markus Meuwly·Nov 13, 2024SaveLearn
Generalized coupled cluster theory for ground and excited state intersectionsCoupled cluster theory in the standard formulation is unable to correctly describe conical intersections among states of the same symmetry. This limitation has restricted the practical application of…Federico Rossi, Eirik F. Kjønstad, Sara Angelico et al.·Nov 13, 2024SaveLearn
Space-local memory in generalized master equations: Reaching the thermodynamic limit for the cost of a small lattice simulationThe exact quantum dynamics of lattice models can be computationally intensive, especially when aiming for large system sizes and extended simulation times necessary to converge transport…Srijan Bhattacharyya, Thomas Sayer, Andrés Montoya-Castillo·Nov 13, 2024SaveLearn
Cholesky Decomposition and the Second-Derivative Two-Electron Integrals Required for the Computation of Magnetizabilities using Gauge-Including Atomic OrbitalsThe computation of magnetizability tensors using gauge-including atomic orbitals is discussed in the context of Cholesky decomposition for the two-electron repulsion integrals with a focus on the…Sophia Burger, Stella Stopkowicz, Jürgen Gauss·Nov 12, 2024SaveLearn