Conditional Wave Function Theory: A Unified Treatment of Molecular Structure 
and Nonadiabatic Dynamics

Albareda Piquer, G.; Lively, K.; Sato, S.; Kelly, A.; Rubio, A.

doi:10.1021/acs.jctc.1c00772

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Conditional Wave Function Theory: A Unified Treatment of Molecular Structure and Nonadiabatic Dynamics

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Albareda Piquer, G.
Nano-Bio Spectroscopy Group and European Theoretical Spectroscopy Facility (ETSF), Universidad del País Vasco (UPV/EHU);
Institute of Theoretical and Computational Chemistry, University of Barcelona;
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Lively, K.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;

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Sato, S.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
Center for Computational Sciences, University of Tsukuba;

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Kelly, A.
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
The Hamburg Centre for Ultrafast Imaging, University of Hamburg;
Department of Chemistry, Dalhousie University, Halifax;

/persons/resource/persons22028

Rubio, A.
Nano-Bio Spectroscopy Group and European Theoretical Spectroscopy Facility (ETSF), Universidad del País Vasco (UPV/EHU);
Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society;
Center for Free-Electron Laser Science;
The Hamburg Centre for Ultrafast Imaging, University of Hamburg;
Center for Computational Quantum Physics (CCQ), Flatiron Institute;

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https://arxiv.org/abs/2107.01094
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https://doi.org/10.1021/acs.jctc.1c00772
(Publisher version)

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Citation

Albareda Piquer, G., Lively, K., Sato, S., Kelly, A., & Rubio, A. (2021). Conditional Wave Function Theory: A Unified Treatment of Molecular Structure and Nonadiabatic Dynamics. Journal of Chemical Theory and Computation, 17(12), 7321-7340. doi:10.1021/acs.jctc.1c00772.

Cite as: https://hdl.handle.net/21.11116/0000-0008-CC51-7

Abstract

We demonstrate that a conditional wave function theory enables a unified and efficient treatment of the equilibrium structure and nonadiabatic dynamics of correlated electron–ion systems. The conditional decomposition of the many-body wave function formally recasts the full interacting wave function of a closed system as a set of lower-dimensional (conditional) coupled “slices”. We formulate a variational wave function ansatz based on a set of conditional wave function slices and demonstrate its accuracy by determining the structural and time-dependent response properties of the hydrogen molecule. We then extend this approach to include time-dependent conditional wave functions and address paradigmatic nonequilibrium processes including strong-field molecular ionization, laser-driven proton transfer, and nuclear quantum effects induced by a conical intersection. This work paves the road for the application of conditional wave function theory in equilibrium and out-of-equilibrium ab initio molecular simulations of finite and extended systems.