Dynamics of Charge-Transfer Processes with Time-Dependent Density Functional 
Theory

Fuks, Johanna I.; Elliott , Peter; Rubio, Angel; Maitra, Neepa T.

doi:10.1021/jz302099f

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Dynamics of Charge-Transfer Processes with Time-Dependent Density Functional Theory

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Rubio, Angel
Nano-Bio Spectroscopy Group, Departamento Fı́sica de Materiales, Universidad del Paı́s Vasco, Centro de Fı́sica de Materiales CSIC-UPV/EHU-MPC and DIPC;
Theory, Fritz Haber Institute, Max Planck Society;

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arXiv:1211.2849
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Citation

Fuks, J. I., Elliott, P., Rubio, A., & Maitra, N. T. (2013). Dynamics of Charge-Transfer Processes with Time-Dependent Density Functional Theory. The Journal of Physical Chemistry Letters, 4(5), 735-739. doi:10.1021/jz302099f.

Cite as: https://hdl.handle.net/11858/00-001M-0000-000E-F3D1-E

Abstract

We show that as an electron transfers between closed-shell molecular
fragments at large separation, the exact correlation potential of
time-dependent density functional theory gradually develops a step and peak
structure in the bonding region. This structure has a density-dependence that
is non-local both in space and time, and even the exact ground-state
exchange-correlation functional fails to cap- ture it. In the complementary
case of charge-transfer between open-shell fragments, an initial step and peak
vanish as the charge-transfer state is reached. Lack of these structures in
usual approxima- tions leads to inaccurate charge-transfer dynamics. This is
dramatically illustrated by the complete lack of Rabi oscillations in the
dipole moment under conditions of resonant charge-transfer.