Field-free molecular orientation induced by single-cycle THz pulses: the role of resonance and quantum interference

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We consider the rotational excitation of molecules induced by asymmetric (“half-cycle”) as well as symmetric single-cycle THz pulses, leading to field-free time-dependent orientation. We show that the basic excitation mechanisms are very similar for the two types of pulses; i.e., the frequency distributions of the pulses at the rotational resonance frequencies play an important role. Furthermore, we investigate the interference between multiple rotational excitation pathways following prealignment with a nonresonant 800-nm femtosecond pulse. It is shown that such interference can lead to an enhancement of the orientation of the linear HCN molecule by a factor close to 2.
Original languageEnglish
JournalPhysical Review A
Issue number1
Pages (from-to)Paper 013408
Number of pages6
Publication statusPublished - 2013

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©2013 American Physical Society

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