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Towards time-dependent current-density-functional theory in the non-linear regime.

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Escartín, JM 
Vincendon, M 
Romaniello, P 
Dinh, PM 
Reinhard, P-G 


Time-Dependent Density-Functional Theory (TDDFT) is a well-established theoretical approach to describe and understand irradiation processes in clusters and molecules. However, within the so-called adiabatic local density approximation (ALDA) to the exchange-correlation (xc) potential, TDDFT can show insufficiencies, particularly in violently dynamical processes. This is because within ALDA the xc potential is instantaneous and is a local functional of the density, which means that this approximation neglects memory effects and long-range effects. A way to go beyond ALDA is to use Time-Dependent Current-Density-Functional Theory (TDCDFT), in which the basic quantity is the current density rather than the density as in TDDFT. This has been shown to offer an adequate account of dissipation in the linear domain when the Vignale-Kohn (VK) functional is used. Here, we go beyond the linear regime and we explore this formulation in the time domain. In this case, the equations become very involved making the computation out of reach; we hence propose an approximation to the VK functional which allows us to calculate the dynamics in real time and at the same time to keep most of the physics described by the VK functional. We apply this formulation to the calculation of the time-dependent dipole moment of Ca, Mg and Na2. Our results show trends similar to what was previously observed in model systems or within linear response. In the non-linear domain, our results show that relaxation times do not decrease with increasing deposited excitation energy, which sets some limitations to the practical use of TDCDFT in such a domain of excitations.



0202 Atomic, Molecular, Nuclear, Particle and Plasma Physics

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J Chem Phys

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AIP Publishing
Engineering and Physical Sciences Research Council (EP/J015059/1)
We thank French research funding agency ANR and Institut Universitaire de France for support during the realization of this work. J.M.E. acknowledges the support of EPSRC Grant No. EP/J015059/1. P.R. and J.M.E. would like to thank J. A. Berger for fruitful discussions.