A5005299370- Spectroscopy and Quantum Chemical Studies
- Advanced Chemical Physics Studies
- Photochemistry and Electron Transfer Studies
- Machine Learning in Materials Science
- Catalysis and Oxidation Reactions
- Molecular spectroscopy and chirality
- Computational Drug Discovery Methods
- Scientific Computing and Data Management
- Electron Spin Resonance Studies
- Free Radicals and Antioxidants
- CO2 Reduction Techniques and Catalysts
- Semiconductor materials and devices
- Advanced Memory and Neural Computing
- Cold Atom Physics and Bose-Einstein Condensates
- Metal complexes synthesis and properties
- Photoreceptor and optogenetics research
- Porphyrin and Phthalocyanine Chemistry
- Spectroscopy and Laser Applications
- Protein Structure and Dynamics
- Inorganic Fluorides and Related Compounds
- Spectroscopy Techniques in Biomedical and Chemical Research
- Quantum and electron transport phenomena
- Molecular Junctions and Nanostructures
Microsoft (United States)
2023-2024
Pacific Northwest National Laboratory
2021-2023
Technical University of Munich
2023
ETH Zurich
2023
Microsoft (Switzerland)
2023
Microsoft (Norway)
2022-2023
University of Minnesota
2016-2022
Jilin University
2016-2022
Shenzhen Bay Laboratory
2020-2022
University of Washington
2020-2022
A multistate density functional theory (MSDFT) is presented in which the energies and densities for ground excited states are treated on same footing using multiconfigurational approaches. The method can be applied to systems with strong correlation correctly describe dimensionality of conical intersections between strongly coupled dissociative potential energy surfaces. dynamic-then-static framework treating electron developed first incorporate dynamic into contracted state functions...
Quantum chemical calculations on atomistic systems have evolved into a standard approach to studying molecular matter. These often involve significant amount of manual input and expertise, although most this effort could be automated, which would alleviate the need for expertise in software hardware accessibility. Here, we present AutoRXN workflow, an automated workflow exploratory high-throughput electronic structure systems, (i) density functional theory methods are exploited deliver...
We describe a diabatic-at-construction (DAC) strategy for defining diabatic states to determine the adiabatic ground and excited electronic their potential energy surfaces using multistate density functional theory (MSDFT). The DAC approach differs in two fundamental ways from adiabatic-to-diabatic (ATD) procedures that transform set of preselected new representation. (1) are defined first computation step form an active space, whose configuration interaction produces second MSDFT. Thus,...
Kohn–Sham density functional theory has been tremendously successful in chemistry and physics. Yet, it is unable to describe the energy degeneracy of spin-multiplet components with any approximate functional. This work features two contributions. (1) We present a multistate (MSDFT) represent determine multiplet energies. MSDFT hybrid approach, taking advantage both wave function theory. Thus, functions, electron densities density-functionals for ground excited states different are treated on...
Delta self-consistent-field methods are widely used in studies of electronically excited states. However, the nonaufbau determinants generally spin-contaminated. Here, we describe a general approach for spin-coupling interactions open-shell molecules, making use multistate density functional theory (MSDFT). In particular, effective exchange integrals that determine spin coupling obtained by enforcing multiplet degeneracy S+1 state MS = S manifold. Consequently, they consistent with energy...
The block-localized wave function method is useful to provide insights on chemical bonding and intermolecular interactions through energy decomposition analysis. relies block localization of molecular orbitals (MOs) by constraining the basis functions within given blocks. Here, a generalized orbital (GBLO) described allow both physically localized delocalized MOs be constrained in orbital-block definitions. Consequently, GBLO optimization can conveniently tailored imposing specific...
Vibrational spectroscopy is a useful technique for probing chemical environments. The development of models that can reproduce the spectra nitriles and azides valuable because these probes are uniquely suited investigating complex systems. Empirical vibrational spectroscopic maps commonly employed to obtain instantaneous frequencies during molecular dynamics simulations but often fail adequately describe behavior probes, especially in its transferability diverse range In this paper, we...
A procedure, called generalized diabatic-at-construction (GDAC), is presented to transform adiabatic potential energy surfaces into a diabatic representation by singular value decomposition. First, we use set of localized, valence bond-like configuration state functions, DAC, as the basis states. Then, ground and relevant excited states are determined using multistate density functional theory (MSDFT). GDAC differs in opposite direction from traditional approaches based on...
Linear and two-dimensional infrared (IR) spectroscopy of site-specific probe molecules provides an opportunity to gain a molecular-level understanding the local hydrogen-bonding network, conformational dynamics, long-range electrostatic interactions in condensed-phase biological systems. A challenge computation is determine time-dependent vibrational frequencies that incorporate explicitly both nuclear quantum effects motions electronic structural representation potential energy surface. In...
The transformative impact of modern computational paradigms and technologies, such as high-performance computing (HPC), quantum computing, cloud has opened up profound new opportunities for scientific simulations. Scalable chemistry is one beneficiary this technological progress. main focus paper on the performance various chemical formulations, ranging from low-order methods to high-accuracy approaches, implemented in different packages libraries, NWChem, NWChemEx, Predictive Methods...
Fourier transform infrared and two-dimensional IR (2D-IR) spectroscopies were applied to two different silanes in three solvents. The selected solutes exhibit degrees of vibrational solvatochromism for the Si–H vibration. Density functional theory calculations confirm that this difference sensitivity is result higher mode polarization with more electron withdrawing ligands. This also affects extent spectral diffusion experienced by silane vibration, offering a potential route simultaneously...
Molecular dynamics simulation of human heart lactate dehydrogenase (LDH) has been carried out to determine the linear and two-dimensional Fourier transform infrared (2D-FTIR) spectra for carbonyl stretch vibration pyruvate in tetrameric enzyme, using quantum vibrational perturbation theory. The computed line-shapes individual subunits are inhomogeneously broadened span entire absorption range full indicating similar conformation heterogeneity four active sites LDH. However, each subunit...
In this article, we develop a relativistic exact-two-component nonorthogonal configuration interaction (X2C-NOCI) for computing L-edge X-ray spectra. This article to our knowledge is the first time NOCI has been used wave functions. A set of molecular complexes, including SF6, SiCl4 and [FeCl6]3-, are demonstrate accuracy computational scaling X2C-NOCI method. Our results suggest that able satisfactorily capture main features L2,3-edge absorption Excitations from core require large amount...
Quantum chemical calculations on atomistic systems have evolved into a standard approach to study molecular matter. These often involve significant amount of manual input and expertise although most this effort could be automated, which would alleviate the need for in software hardware accessibility. Here, we present AutoRXN workflow, an automated workflow exploratory high-throughput lectronic structure systems, (i) density functional theory methods are exploited deliver minimum...
Variational energy decomposition analyses have been presented to quantify the σ-dative, ligand-to-metal forward charge transfer (CT) and π-conjugative, metal-to-ligand backward delocalization on a series of isolelectronic transition-metal carbonyl complexes M(CO)6, including M = Ti2–, V–, Cr, Mn+, Fe2+. Although qualitative features these terms are understood, well-defined quantitative studies scarce. Consistent with early findings, electrostatic Pauli exchange effects play key role in...
Block-localized wave function is a useful method for optimizing constrained determinants. In this article, we extend the generalized block-localized technique to relativistic two-component framework. Optimization of excited state determinants functions presents unique challenge because manifold often quite dense with degenerate states. Furthermore, test degree which certain symmetries result naturally from ΔSCF optimization such as time-reversal symmetry and respect total angular momentum...
The quantitative prediction of vibrational spectra chromophore molecules in solution is challenging and numerous methods have been developed. In this work, we present a quantum vibration perturbation (QVP) approach, which procedure that combines molecular dynamics with theory. framework, an initial Newtonian simulation performed, followed by substitution process to embed wave functions into the trajectory. instantaneous frequency shift at each time step calculated using Rayleigh-Schrödinger...
This is the data and associated new software required to run multi-state density-functional theory (MSDDFT) calculations by GAMESS programme. Also, needed drive based on output from Gaussian-16 package included. Sample input files are included, as well Perl scripts Fortran source code. A separate execution of create specifications for each state be included in MSDFT, then after more calculate final energies. The basic results described "Multistate density functional applied with 3 unpaired...