Generic Mechanism of Optimal Energy Transfer Efficiency: A Scaling Theory of the Mean First-Passage Time in Exciton Systems

Jianlan Wu, Robert J. Silbey, and Jianshu Cao
Phys. Rev. Lett. 110, 200402 – Published 13 May 2013

Abstract

An asymptotic scaling theory is presented using the conceptual basis of trapping-free subspace (i.e., orthogonal subspace) to establish the generic mechanism of optimal efficiency of excitation energy transfer in light-harvesting systems. A quantum state orthogonal to the trap will exhibit noise-assisted transfer, clarifying the significance of initial preparation. For such an initial state, the efficiency is enhanced in the weak damping limit (t1/Γ), and suppressed in the strong damping limit (tΓ), analogous to Kramers turnover in classical rate theory. An interpolating expression t=A/Γ+B+CΓ quantitatively describes the trapping time over the entire range of the dissipation strength, and predicts the optimal efficiency at ΓoptJ for homogenous systems. In the presence of static disorder, the scaling law of transfer time with respect to dephasing rate changes from linear to square root, suggesting a weaker dependence on the environment. The prediction of the scaling theory is verified in a symmetric dendrimer system by numerically exact quantum calculations. Though formulated in the context of excitation energy transfer, the analysis and conclusions apply in general to open quantum processes, including electron transfer, fluorescence emission, and heat conduction.

  • Received 16 November 2010

DOI:https://doi.org/10.1103/PhysRevLett.110.200402

© 2013 American Physical Society

Authors & Affiliations

Jianlan Wu1,2, Robert J. Silbey1,*, and Jianshu Cao1,†

  • 1Department of Chemistry, MIT, 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, USA
  • 2Physics Department, Zhejiang University, 38 ZheDa Road, Hangzhou, Zhejiang 310027, China

  • *Deceased.
  • jianshu@mit.edu

Article Text (Subscription Required)

Click to Expand

References (Subscription Required)

Click to Expand
Issue

Vol. 110, Iss. 20 — 17 May 2013

Reuse & Permissions
Access Options
CHORUS

Article Available via CHORUS

Download Accepted Manuscript
Author publication services for translation and copyediting assistance advertisement

Authorization Required


×
×

Images

×

Sign up to receive regular email alerts from Physical Review Letters

Log In

Cancel
×

Search


Article Lookup

Paste a citation or DOI

Enter a citation
×