Speaker
Description
Fewest-switches surface hopping (FSSH) is one of the most popular methods for simulating photochemical experiments [1], even though it suffers from problems of inconsistency and overcoherence that significantly degrade the accuracy of its results. In particular, FSSH is unable to correctly describe the dynamics under strong electromagnetic pulses [2,3], such that a fully satisfactory approach for simulating the photoexcitation step of many experiments is currently lacking.
The mapping approach to surface hopping (MASH) [4] is a recently developed method that alleviates the problems of FSSH at no additional cost. Through application to experimentally relevant photochemical systems, I will demonstrate that the MASH algorithm can successfully treat the dynamics involving strong explicit laser pulses, including off-resonant excitation processes.
[1] J. E. Subotnik et al., Annu. Rev. Phys. Chem., 67, 387, (2016)
[2] T. Fiedlschuster, et al., Phys. Rev. A, 95, 063424 (2017)
[3] B. Mingolet, B. F. E. Curchod, J. Phys. Chem. A, 123, 3582-3591 (2019)
[4] J. R. Mannouch, J. O. Richardson, J. Chem. Phys. 158, 10411 (2023)
