Published November 24, 2011 | Version v1
Journal article

Time-dependent density-functional and reduced density-matrix methods for few electrons: Exact versus adiabatic approximations

  • 1. European Theoretical Spectroscopy Facility (Country Unknown)
  • 2. Nano-Bio Spectroscopy group, Dpto. Física de Materiales, Universidad del País Vasco, Centro de Física de Materiales CSIC-UPV/EHU-MPC and DIPC, Av. Tolosa 72, E-20018 San Sebastián (Spain)
  • 3. IKERBASQUE, Basque Foundation for Science, E-48011 Bilbao (Spain)
  • 4. Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin (Germany)
  • 5. Max-Planck-Institut für Mikrostrukturphysik, Weinberg 2, D-06120 Halle (Germany)

Description

Graphical abstract: We solve a 1D N-electron system, with N small, by mapping it onto an N-dimensional one-electron problem. We compare the exact solutions to the results from adiabatic density and density matrix functionals for different physical situations. Highlights: ► Static and dynamical correlations. ► Memory dependence of exchange-correlation functionals in TDDFT. ► Linear and non-linear response. ► Laser-induced population control. - Abstract: To address the impact of electron correlations in the linear and non-linear response regimes of interacting many-electron systems exposed to time-dependent external fields, we study one-dimensional (1D) systems where the interacting problem is solved exactly by exploiting the mapping of the 1D N-electron problem onto an N-dimensional single electron problem. We analyze the performance of the recently derived 1D local density approximation as well as the exact-exchange orbital functional for those systems. We show that the interaction with an external resonant laser field shows Rabi oscillations which are detuned due to the lack of memory in adiabatic approximations. To investigate situations where static correlations play a role, we consider the time-evolution of the natural occupation numbers associated to the reduced one-body density matrix. Those studies shed light on the non-locality and time-dependence of the exchange and correlation functionals in time-dependent density and density-matrix functional theories.

Availability note (English)

Available from http://dx.doi.org/10.1016/j.chemphys.2011.06.010

Additional details

Identifiers

DOI
10.1016/j.chemphys.2011.06.010;
arXiv
arXiv:1108.3196v1;
PII
S0301-0104(11)00248-5;

Publishing Information

Journal Title
Chemical Physics
Journal Volume
391
Journal Issue
1
Journal Page Range
p. 1-10
ISSN
0301-0104
CODEN
CMPHC2

Optional Information

Copyright
Copyright (c) 2011 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.