期刊
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
卷 17, 期 1, 页码 29-39出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.0c01035
关键词
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资金
- US Department of Energy, Office of Basic Energy Sciences [DE-SC0020437]
- National Science Foundation [CHE-1955407]
- U.S. Department of Energy (DOE) [DE-SC0020437] Funding Source: U.S. Department of Energy (DOE)
The newly developed method incorporates a classical external electromagnetic field into nonadiabatic dynamics, allowing for the description of field-driven dynamics and computation of various linear and nonlinear spectroscopic signals. By applying this method to a simple model, the impact of different pulse shapes on experimental signals was explored.
The partially linearized density matrix formalism for nonadiabatic dynamics is adapted to incorporate a classical external electromagentic field into the system Hamiltonian. This advancement encompasses the possibility of describing field-driven dynamics and computing a variety of linear and nonlinear spectroscopic signals beyond the perturbative limit. The capabilities of the developed approach are demonstrated on a simple two-state vibronic model coupled to a bath, for which we (a) perform an exhaustive search in the field parameter space for optimal state preparation and (b) compute time-resolved transient absorption spectroscopy to monitor the effect of different pulse shapes on measurable experimental signals. While no restrictions on the form of the field have to be assumed, we focus here on Gaussian shaped (linearly) chirped pulses.
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