Time-dependent density functional theory scheme for efficient calculations of dynamic (hyper)polarizabilities.
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.
Andrade
Xavier
X
Departamento de Física de Materiales, Facultad de Ciencias Químicas, UPV/EHU Centro Mixto CSIC-UPV/EHU and European Theoretical Spectroscopy Facility (ETSF), E-20018 San Sebastián, Spain. xavier@tddft.org
Botti
Silvana
S
Marques
Miguel A L
MA
Rubio
Angel
A