Origin of symmetry-forbidden high-order harmonic generation in the time-dependent Kohn-Sham formulation

Xiaoning Zang; Ce Shang; Pengcheng Zhang; Yalei Zhu; Zhiyong Zhu; Udo Schwingenschlögl

doi:10.1103/PhysRevA.103.043106

Origin of symmetry-forbidden high-order harmonic generation in the time-dependent Kohn-Sham formulation

Xiaoning Zang, Ce Shang, Pengcheng Zhang, Yalei Zhu, Zhiyong Zhu, Udo Schwingenschlögl

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2 Scopus citations

Abstract

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.

Original language	English (US)
Journal	Physical Review A
Volume	103
Issue number	4
DOIs	https://doi.org/10.1103/PhysRevA.103.043106
State	Published - Apr 12 2021

Bibliographical note

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.

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title = "Origin of symmetry-forbidden high-order harmonic generation in the time-dependent Kohn-Sham formulation",

abstract = "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.",

author = "Xiaoning Zang and Ce Shang and Pengcheng Zhang and Yalei Zhu and Zhiyong Zhu and Udo Schwingenschl{\"o}gl",

note = "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 Aur{\'e}lien Manchon for helpful discussions.",

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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.

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JO - Physical Review A

JF - Physical Review A

IS - 4

ER -

Origin of symmetry-forbidden high-order harmonic generation in the time-dependent Kohn-Sham formulation

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