
doi: 10.1063/1.2136155
pmid: 16392930
Optimal control theory is employed for the task of minimizing the excited-state population of a dye molecule in solution. The spectrum of the excitation pulse is contained completely in the absorption band of the molecule. Only phase control is studied which is equivalent to optimizing the transmission of the pulse through the medium. The molecular model explicitly includes two electronic states and a single vibrational mode. The other degrees of freedom are classified as bath modes. The surrogate Hamiltonian method is employed to incorporate these bath degrees of freedom. Their influence can be classified as electronic dephasing and vibrational relaxation. In accordance with experimental results, minimal excitation is associated with a negatively chirped pulses. Optimal pulses with more complex transient structure are found to be superior to linearly chirped pulses. The difference is enhanced when the fluence is increased. The improvement degrades when dissipative effects become more dominant.
| selected citations These citations are derived from selected sources. This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically). | 10 | |
| popularity This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network. | Average | |
| influence This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically). | Average | |
| impulse This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network. | Top 10% |
