Mechanism of Molecular Orientation by Single-cycle Pulses

Abstract

Significant molecular orientation can be achieved by time-symmetric single-cycle pulses of zero area, in the THz region. We show that in spite of the existence of a combined time-space symmetry operation, not only large peak instantaneous orientations but also nonzero time-average orientations over a rotational period can be obtained. We show that this unexpected phenomenon is due to interferences among eigenstates of the time-evolution operator, as was described previously for transport phenomena in quantum ratchets. This mechanism also works for sequences of identical pulses, spanning a rotational period. This fact can be used to obtain a net average molecular orientation regardless of the magnitude of the rotational constant.

Published version may be found at (URL:http://link.aip.org/link?/JCP/137/044303). Substantial changes with respect to previous versions, including new title

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Cited by in corpus (11)

• Quantum control of molecular rotation
• On the observation of field-free orientation of a symmetric top molecule by terahertz laser pulses at high temperature
• Optimal three-state field-free molecular orientation with terahertz pulses
• Orientational quantum revivals induced by a single-cycle terahertz pulse
• Coherent radiative decay of molecular rotations: a comparative study of terahertz-oriented versus optically aligned molecular ensembles
• Control of molecular dynamics with zero-area fields: Application to molecular orientation and photofragmentation
• Shaping of the time-evolution of field-free molecular orientation by THz laser pulses
• Orientation and Alignment Dynamics of Polar Molecule Driven by Shaped Laser Pulses
• Theoretical study of asymmetric superrotors: alignment and orientation
• Unified parameter for localization in isotope-selective rotational excitation of diatomic molecules using a train of optical pulses
• External constraints on optimal control strategies in molecular orientation and photofragmentation: Role of zero-area fields