| Title |
Efficient Kohn-Sham density-functional theory implementation of isotropic spectroscopic observables associated with quadratic response functions / |
| Authors |
Ahmadzadeh, Karan ; Li, Xin ; Rinkevicius, Zilvinas ; Norman, Patrick |
| DOI |
10.1088/2516-1075/aca859 |
| Full Text |
|
| Is Part of |
Electronic structure.. Bristol : Institute of physics. 2022, vol. 4, iss. 4, art. no. 044004, p. 1-23.. ISSN 2516-1075 |
| Keywords [eng] |
density functional theory ; nonlinear optics ; response theory |
| Abstract [eng] |
For general exchange-correlation functionals with a dependence on the local spin densities and spin-density gradients, we provide computationally tractable expressions for the tensor-averaged quadratic response functions pertinent to the experimental observables in second-harmonic generation (SHG). We demonstrate how the tensor-averaged quantities can be implemented with reference to a derived minimal number of first- and second-order perturbed Fock matrices. Our consideration has the capability of treating a situation of resonance enhancement as it is based on damped response theory and allows for the evaluation of tensor-averaged resonant-convergent quadratic response functions using only ∼25% (one-photon off-resonance regions) and ∼50% (one-photon resonance regions) of the number of auxiliary Fock matrices required when explicitly calculating all the needed individual tensor components. Numerical examples of SHG intensities in the one-photon off-resonance region are provided for a sample of makaluvamine derivatives recognized for their large nonlinear optical responses as well as a benchmark set of small- and medium-sized organic molecules. |
| Published |
Bristol : Institute of physics |
| Type |
Journal article |
| Language |
English |
| Publication date |
2022 |
| CC license |
|
