Maximum attainable field-free molecular orientation of a thermal ensemble with near-single-cycle THz pulses

Sheng Lun Liao, Tak San Ho, Herschel Rabitz, Shih I. Chu

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Abstract

Recently, single-cycle THz pulses have been demonstrated in the laboratory to successfully induce field-free orientation in gas-phase polar molecules at room temperature. In this paper, we examine the maximum attainable field-free molecular orientation with optimally shaped linearly polarized near-single-cycle THz laser pulses of a thermal ensemble. Large-scale benchmark optimal control simulations are performed, including rotational energy levels with the rotational quantum numbers up to J=100 for OCS linear molecules. The simulations are made possible by an extension of the recently formulated fast search algorithm, the two-point boundary-value quantum control paradigm, to the mixed-states optimal control problems in the present work. It is shown that a very high degree of field-free orientation can be achieved by strong, optimally shaped near-single-cycle THz pulses. The extensive numerical simulations showed that the maximum attainable J-dependent field-free orientation (equal to 0.714 for J=60 and 0.837 for J=100 at 100 K) in the near-single-cycle THz pulse region is close to 92% of the corresponding optimal bound that can be attained by arbitrarily long pulses. It is also found that a smaller amplitude for the optimal control field corresponds to a smaller J (e.g., ≈0.005 a.u. for J=60 and ≈0.01 a.u. for J=100) in the model simulations. The latter finding may underline the actual experimental performance of the field-free molecular orientation, since presently the available amplitude of single-cycle THz pulses can only reach slightly beyond 20MV/cm (≈0.0038 a.u.).

Original languageEnglish (US)
Article number013429
JournalPhysical Review A - Atomic, Molecular, and Optical Physics
Volume87
Issue number1
DOIs
StatePublished - Jan 25 2013

All Science Journal Classification (ASJC) codes

  • Atomic and Molecular Physics, and Optics

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