Liao Sheng-Lun, Ho Tak-San, Rabitz Herschel, Chu Shih-I
Center for Quantum Science and Engineering and Department of Physics, National Taiwan University, Taipei 10617, Taiwan.
Department of Chemistry, Princeton University, Princeton, New Jersey 08544, USA.
Phys Rev Lett. 2017 Jun 16;118(24):243001. doi: 10.1103/PhysRevLett.118.243001.
A long-standing challenge in the time-dependent density functional theory is to efficiently solve the exact time-dependent optimized effective potential (TDOEP) integral equation derived from orbital-dependent functionals, especially for the study of nonadiabatic dynamics in time-dependent external fields. In this Letter, we formulate a completely equivalent time-local TDOEP equation that admits a unique real-time solution in terms of time-dependent Kohn-Sham and effective memory orbitals. The time-local formulation is numerically implemented, with the incorporation of exponential memory loss to address the unaccounted for correlation component in the exact-exchange-only functional, to enable the study of the many-electron dynamics of a one-dimensional hydrogen chain. It is shown that the long time behavior of the electric dipole converges correctly and the zero-force theorem is fulfilled in the current implementation.
