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Title: Time-dependent potential-functional embedding theory

We introduce a time-dependent potential-functional embedding theory (TD-PFET), in which atoms are grouped into subsystems. In TD-PFET, subsystems can be propagated by different suitable time-dependent quantum mechanical methods and their interactions can be treated in a seamless, first-principles manner. TD-PFET is formulated based on the time-dependent quantum mechanics variational principle. The action of the total quantum system is written as a functional of the time-dependent embedding potential, i.e., a potential-functional formulation. By exploiting the Runge-Gross theorem, we prove the uniqueness of the time-dependent embedding potential under the constraint that all subsystems share a common embedding potential. We derive the integral equation that such an embedding potential needs to satisfy. As proof-of-principle, we demonstrate TD-PFET for a Na{sub 4} cluster, in which each Na atom is treated as one subsystem and propagated by time-dependent Kohn-Sham density functional theory (TDDFT) using the adiabatic local density approximation (ALDA). Our results agree well with a direct TDDFT calculation on the whole Na{sub 4} cluster using ALDA. We envision that TD-PFET will ultimately be useful for studying ultrafast quantum dynamics in condensed matter, where key regions are solved by highly accurate time-dependent quantum mechanics methods, and unimportant regions are solved by faster, less accurate methods.
Authors:
 [1] ;  [2] ;  [3] ;  [4]
  1. Theoretical Division, Los Alamos National Laboratory, New Mexico 87544 (United States)
  2. Institute for Theoretical Physics, Vienna University of Technology, Wiedner Hauptstra├če 8-10/136, 1040 Vienna (Austria)
  3. Department of Mechanical, Aerospace and Nuclear Engineering, Rensselaer Polytechnic Institute, Troy, New York 12180 (United States)
  4. Department of Mechanical and Aerospace Engineering and Chemistry, Program in Applied and Computational Mathematics, and Andlinger Center for Energy and the Environment, Princeton University, Princeton, New Jersey 08544 (United States)
Publication Date:
OSTI Identifier:
22253357
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 12; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; APPROXIMATIONS; DENSITY; DENSITY FUNCTIONAL METHOD; INTEGRAL EQUATIONS; POTENTIALS; TIME DEPENDENCE