Analytical formulation of the second-order derivative of energy for orbital-optimized variational quantum eigensolver: application to polarizabilityWe develop a quantum-classical hybrid algorithm to calculate the analytical second-order derivative of the energy for the orbital-optimized variational quantum eigensolver (OO-VQE), which is a method…Yuya O. Nakagawa, Jiabao Chen, Shotaro Sudo et al.·Nov 7, 2022SaveLearn
Direct deduction of chemical class from NMR spectraThis paper presents a proof-of-concept method for classifying chemical compounds directly from NMR data without doing structure elucidation. This can help to reduce time in finding good structure…Stefan Kuhn, Carlos Cobas, Agustin Barba et al.·Nov 6, 2022SaveLearn
Is explicitly correlated double hybrid DFT advantageous for vibrational frequencies?We have investigated the effect of F12 geminals on the basis set convergence of harmonic frequencies calculated using two representative double-hybrid density functionals, namely B2GP-PLYP and…Nisha Mehta, Golokesh Santra, Jan M. L. Martin·Nov 6, 2022SaveLearn
Improved torque estimator for condensed-phase quasicentroid molecular dynamicsWe describe improvements to the quasicentroid molecular dynamics (QCMD) path-integral method, which was developed recently for computing the infrared spectra of condensed-phase systems. The main…George Trenins, Christopher Haggard, Stuart C. Althorpe·Nov 6, 2022SaveLearn
State-Specific Configuration Interaction for Excited StatesWe introduce and benchmark a systematically improvable route for excited-state calculations, state-specific configuration interaction (), which is a particular realization of…Fábris Kossoski, Pierre-François Loos·Nov 6, 2022SaveLearn
An efficient electrostatic embedding QM/MM method using periodic boundary conditions based on particle-mesh Ewald sums and electrostatic potential fitted charge operatorsHybrid quantum mechanics / molecular mechanics (QM/MM) models successfully describe the properties of biological macromolecules. However, most QM/MM methodologies are constrained to unrealistic gas…Simone Bonfrate, Nicolas Ferré, Miquel et al.·Nov 4, 2022SaveLearn
Ultrasensitive Surface-Enhanced Raman Spectroscopy Detection by Porous Silver Supraparticles from Self-Lubricating Drop EvaporationThis work demonstrates an original and ultrasensitive approach for surface-enhanced Raman spectroscopy (SERS) detection based on evaporation of self-lubricating drops containing silver…Tulsi Satyavir Dabodiya, Somasekhara Goud Sontti, Zixiang Wei et al.·Nov 4, 2022SaveLearn
A Universal Method for Analysing Copolymer GrowthPolymers consisting of more than one type of monomer, known as copolymers, are vital to both living and synthetic systems. Copolymerisation has been studied theoretically in a number of contexts,…Benjamin J. Qureshi, Jordan Juritz, Jenny M. Poulton et al.·Nov 4, 2022SaveLearn
Non-Linear Correlation Functions and Zero-Point Energy Flow in Mixed Quantum-Classical Semiclassical DynamicsMixed Quantum Classical (MQC)-IVR is a recently introduced semiclassical framework that allows for selective quantization of the modes of a complex system. In the quantum limit, MQC reproduces the…Shreyas Malpathak, Nandini Ananth·Nov 4, 2022SaveLearn
Cavity-free continuum solvation: implementation and parametrization in a multiwavelet frameworkWe present a multiwavelet-based implementation of a quantum/classical polarizable continuum model. The solvent model uses a diffuse solute-solvent boundary and a position-dependent permittivity,…Gabriel A. Gerez S., Roberto Di Remigio Eikås, Stig Rune Jensen et al.·Nov 4, 2022SaveLearn
The Bethe-Salpeter QED wave equation for bound-state computations of atoms and moleculesInteractions in atomic and molecular systems are dominated by electromagnetic forces and the theoretical framework must be in the quantum regime. The physical theory for the combination of quantum…Edit Mátyus, Dávid Ferenc, Péter Jeszenszki et al.·Nov 4, 2022SaveLearn
Complementary experimental methods to obtain thermodynamic parameters of protein ligand systemsIn recent years, thermophoresis has emerged as a promising tool for quantifying biomolecular interactions. The underlying physical effect is still not understood. To gain deeper insight, we…Shilpa Mohanakumar, Namkyu Lee, Simone Wiegand·Nov 4, 2022SaveLearn
Excited-state molecular dynamics simulation based on variational quantum algorithmsWe propose an excited-state molecular dynamics simulation method based on variational quantum algorithms at a computational cost comparable to that of ground-state simulations. We utilize the feature…Hirotoshi Hirai·Nov 4, 2022SaveLearn
Photoexcited state dynamics and singlet fission in carotenoidsWe describe our dynamical simulations of the excited states of the carotenoid, neurosporene, following its photoexcitation into the 'bright' (nominally 11Bu+) state. We employ the adaptive tDMRG…Dilhan Manawadu, Timothy N. Georges, William Barford·Nov 4, 2022SaveLearn
Beat-frequency-resolved two-dimensional electronic spectroscopy: disentangling vibrational coherences in artificial fluorescent proteins with sub-10-fs visible laser pulsesWe perform a beat-frequency-resolved analysis for two-dimensional electronic spectroscopy using a high-speed and stable 2D electronic spectrometer and few-cycle visible laser pulses to disentangle…Masaaki Tsubouchi, Nobuhisa Ishii, Yuji Kagotani et al.·Nov 4, 2022SaveLearn
Femtosecond intramolecular rearrangement of the CH3NCS radical cationStrong-field ionization, involving tunnel ionization and electron rescattering, enables femtosecond time-resolved dynamics measurements of chemical reactions involving radical cations. Here, we…Jacob Stamm, Shuai Li, Bethany Jochim et al.·Nov 3, 2022SaveLearn
Comparison of Matsubara dynamics with exact quantum dynamics for an oscillator coupled to a dissipative bathMatsubara dynamics is the classical dynamics which results when imaginary-time path-integrals are smoothed; it conserves the quantum Boltzmann distribution and appears in drastically approximated…Adam Prada, Eszter S. Pós, Stuart C. Althorpe·Nov 3, 2022SaveLearn
Dynamical simulations of carotenoid photoexcited states using density matrix renormalization group techniquesWe present a dynamical simulation scheme to model the highly correlated excited state dynamics of linear polyenes. We apply it to investigate the internal conversion processes of carotenoids…Dilhan Manawadu, Darren J. Valentine, William Barford·Nov 3, 2022SaveLearn
Transition dynamics and metastable states during premelting and freezing of ice surfacesThe premelting of ice is well known, but little is known about how the premelted and solid surfaces convert to each other. In this work, the transition dynamics between two phases are revealed with…Shifan Cui, Haoxiang Chen·Nov 3, 2022SaveLearn
Technologies to Capture CO2 directly from Ambient AirBuilding a carbon-neutral world needs to remove the excess CO2 that has already been dumped into the atmosphere. The sea, soil, vegetation, and rocks on Earth all naturally uptake CO2 from the…Gahyun Annie Lee, Xiaoyang Shi, Ah-Hyung Alissa Park·Nov 2, 2022SaveLearn
Atom-Specific Probing of Electron Dynamics in an Atomic Adsorbate by Time-Resolved X-ray SpectroscopyThe electronic excitation occurring on adsorbates at ultrafast time scales from optical lasers that initiate surface chemical reactions is still an open question. Here, we report the ultrafast…Simon Schreck, Elias Diesen, Martina Dell'Angela et al.·Nov 1, 2022SaveLearn
A configuration interaction correction on top of pair coupled cluster doublesNumerous numerical studies have shown that geminal-based methods are a promising direction to model strongly correlated systems with low computational costs. Several strategies have been introduced…Artur Nowak, Katharina Boguslawski·Nov 1, 2022SaveLearn
Grid-based state space exploration for molecular bindingBinding processes are difficult to sample with molecular-dynamics (MD) simulations. In particular, the state space exploration is often incomplete. Evaluating the molecular interaction energy on a…Hana Zupan, Frederick Heinz, Bettina G. Keller·Nov 1, 2022SaveLearn
Noise and Thermodynamic Uncertainty Relation in "Underwater" Molecular JunctionsWe determine the zero-frequency charge current noise in a metal-molecule-metal junction embedded in a thermal environment, e.g., a solvent, dominated by sequential charge transmission described by a…Henning Kirchberg, Abraham Nitzan·Oct 31, 2022SaveLearn
Density Matrix Renormalization Group for Transcorrelated Hamiltonians: Ground and Excited States in ab initio SystemsWe present the theory of a density matrix renormalization group (DMRG) algorithm which can solve for both the ground and excited states of non-Hermitian transcorrelated Hamiltonians, and show…Ke Liao, Huanchen Zhai, Evelin Martine Christlmaier et al.·Oct 31, 2022SaveLearn