Modified Scaled Hierarchical Equation of Motion Approach for the Study of Quantum Coherence in Photosynthetic Complexes

Jing Zhu, Birck Nanotechnology Center, Purdue University
Sabre Kais, Birck Nanotechnology Center, Purdue University
Patrick Rebentrost, Purdue University
Alan Aspuru-Guzik, Purdue University

Date of this Version



J. Phys. Chem. B, 2011, 115 (6), pp 1531–1537


We present a detailed theoretical study of the transfer of electronic excitation energy through the Fenna-Matthews-Olson (FMO) pigment-protein complex, using the newly developed modified scaled hierarchical approach (Shi, Q; et al. J. Chem. Phys. 2009, 130, 084105). We show that this approach is computationally more efficient than the original hierarchical approach. The modified approach reduces the truncation levels of the auxiliary density operators and the correlation function. We provide a systematic study of how the number of auxiliary density operators and the higher-order correlation functions affect the exciton dynamics. The time scales of the coherent beating are consistent with experimental observations. Furthermore, our theoretical results exhibit population beating at physiological temperature. Additionally, the method does not require a low-temperature correction to obtain the correct thermal equilibrium at long times.


Nanoscience and Nanotechnology