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Time-dependent density functional theory scheme for efficient calculations of dynamic (hyper)polarizabilities

X. Andrade, S. Botti, M. Marques, A. Rubio

The Journal of Chemical Physics, 126, 184106, (2007)

DOI: 10.1063/1.2733666

Download: BibTEX

The authors present an efficient perturbative method to obtain both static and dynamic polarizabilities and hyperpolarizabilities of complex electronic systems. This approach is based on the solution of a frequency-dependent Sternheimer equation, within the formalism of time-dependent density functional theory, and allows the calculation of the response both in resonance and out of resonance. Furthermore, the excellent scaling with the number of atoms opens the way to the investigation of response properties of very large molecular systems. To demonstrate the capabilities of this method, they implemented it in a real-space (basis-set-free) code and applied it to benchmark molecules, namely, CO, H2O⁠, and para-nitroaniline. Their results are in agreement with experimental and previous theoretical studies and fully validate their approach.

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{"type":"article", "name":"x.andrade20075", "author":"X. Andrade and S. Botti and M. Marques and A. Rubio", "title":"Timedependent density functional theory scheme for efficient calculations of dynamic (hyper)polarizabilities", "journal":"The Journal of Chemical Physics", "volume":"126", "OPTnumber":"18", "OPTmonth":"5", "year":"2007", "OPTpages":"184106", "OPTnote":"", "OPTkey":"exchange correlation functionals; local density approximations; Kohn-Sham equation; time dependent density functional theory; phonons; algorithms and data structure; hyperpolarizability, Polarizability, Second harmonic generation, Adiabatic theorem", "DOI":"10.1063/1.2733666"}
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