TY - JOUR
T1 - Origin of symmetry-forbidden high-order harmonic generation in the time-dependent Kohn-Sham formulation
AU - Zang, Xiaoning
AU - Shang, Ce
AU - Zhang, Pengcheng
AU - Zhu, Yalei
AU - Zhu, Zhiyong
AU - Schwingenschlögl, Udo
N1 - KAUST Repository Item: Exported on 2021-04-30
Acknowledgements: We acknowledge financial support from King Abdullah University of Science and Technology (KAUST). For computer time, this research used the resources of the Supercomputing Laboratory at KAUST. We thank Nicolas Tancogne-Dejean and Aurélien Manchon for helpful discussions.
PY - 2021/4/12
Y1 - 2021/4/12
N2 - We find, for two-electron closed-shell systems (H2 molecule, He atom), symmetry-forbidden peaks in the high-order harmonic spectra obtained by the time-dependent Kohn-Sham equations, and clarify their origin. It turns out that fixation of the number of Kohn-Sham orbitals and their occupations gives rise to unphysical transition paths and, therefore, incorrect populations of the one-electron excited states, which leads to even-order harmonics in systems with inversion symmetry. We show that the time-dependent natural Kohn-Sham and time-dependent configuration interaction equations do not suffer from this shortcoming.
AB - We find, for two-electron closed-shell systems (H2 molecule, He atom), symmetry-forbidden peaks in the high-order harmonic spectra obtained by the time-dependent Kohn-Sham equations, and clarify their origin. It turns out that fixation of the number of Kohn-Sham orbitals and their occupations gives rise to unphysical transition paths and, therefore, incorrect populations of the one-electron excited states, which leads to even-order harmonics in systems with inversion symmetry. We show that the time-dependent natural Kohn-Sham and time-dependent configuration interaction equations do not suffer from this shortcoming.
UR - http://hdl.handle.net/10754/669005
UR - https://link.aps.org/doi/10.1103/PhysRevA.103.043106
UR - http://www.scopus.com/inward/record.url?scp=85104437411&partnerID=8YFLogxK
U2 - 10.1103/PhysRevA.103.043106
DO - 10.1103/PhysRevA.103.043106
M3 - Article
SN - 2469-9934
VL - 103
JO - Physical Review A
JF - Physical Review A
IS - 4
ER -