Dissipative electron transfer dynamics in mixed valence dimers: microscopic approach to the solid state problem

Area of Science:

• Physical Chemistry
• Condensed Matter Physics
• Quantum Dynamics

Background:

• Mixed-valence (MV) dimers are crucial in understanding electron transfer processes.
• Low-temperature dynamics are significantly influenced by electron-phonon coupling.
• Existing models often lack microscopic detail for specific dissipative systems.

Purpose of the Study:

• To propose a microscopic analytical approach for low-temperature dissipative electron transfer in MV dimers.
• To investigate the influence of acoustic phonons on electron localization dynamics.
• To explicitly account for relaxation processes without assuming bath spectral functions.

Main Methods:

• Developed a microscopic model coupling MV dimer electrons to acoustic phonons.
• Analyzed the system under conditions of no local modes, weak electron-phonon coupling, and specific energy regimes.
• Calculated time-dependent electron localization probabilities and Rabi oscillation damping.

Main Results:

• Demonstrated super-ohmic dissipation with a spectral function J(ω) ∝ ω(5).
• Observed picosecond-scale damped oscillations in electron localization probabilities.
• Found longitudinal relaxation time T1 to be half the decoherence time T2 (T2 ≤ 2T1).

Conclusions:

• The proposed model accurately describes low-temperature dissipative electron transfer dynamics in MV dimers.
• Electron-phonon coupling leads to significant damping of quantum oscillations.
• The relationship T2 ≤ 2T1 provides an important constraint for understanding relaxation mechanisms.