We introduce a model to investigate electron transfer where the explicit temporal propagation of the electronic wave function is modified by white and colored noises. Atomic energies are perturbed randomly to determine an electron transfer where the periodic electronic oscillations are greatly smothered and the transfer rates can reach up to the experimental time scale. Application to the photolyase enzyme that repairs the DNA lesions shows that the optimal conditions to reproduce the experimental lifetime are equivalent to a red or Brownian noise acting every 80 fs, that is, of ∼400 cm-1. Two-state model calculations show that the results of the quantum dynamics are robust and intrinsic to the use of noise in the simulations.
Fadanni J., Acocella A., Zerbetto F. (2019). White and Colored Noises as Driving Forces of Electron Transfer: The Photolyase Repair Mechanism as a Test Case. THE JOURNAL OF PHYSICAL CHEMISTRY LETTERS, 10(16), 4511-4516 [10.1021/acs.jpclett.9b01763].
White and Colored Noises as Driving Forces of Electron Transfer: The Photolyase Repair Mechanism as a Test Case
Fadanni J.;Acocella A.;Zerbetto F.
2019
Abstract
We introduce a model to investigate electron transfer where the explicit temporal propagation of the electronic wave function is modified by white and colored noises. Atomic energies are perturbed randomly to determine an electron transfer where the periodic electronic oscillations are greatly smothered and the transfer rates can reach up to the experimental time scale. Application to the photolyase enzyme that repairs the DNA lesions shows that the optimal conditions to reproduce the experimental lifetime are equivalent to a red or Brownian noise acting every 80 fs, that is, of ∼400 cm-1. Two-state model calculations show that the results of the quantum dynamics are robust and intrinsic to the use of noise in the simulations.I documenti in IRIS sono protetti da copyright e tutti i diritti sono riservati, salvo diversa indicazione.
