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Chemical Physics Letters

Laser-driven coherent manipulation of molecular chirality

Ioannis Thanopulos, Emmanuel Paspalakis, Z. Kis

Published Apr 29, 2004• 24 citations
Publisher
DOI
10.1016/j.cplett.2004.03.129

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We propose an approach to sensitively probe the chirality of molecules by measuring their coherent optical-absorption spectra. It is shown that quantum dynamics of the cyclic three-level chiral molecules driven by appropriately designed external fields is total-phase dependent. This will result in chirality-dependent absorption spectra for the probe field. As a consequence, the charality-dependent information in the spectra (such as the locations and relative heights of the characteristic absorption peaks) can be utilized to identify molecular chirality and determinate enantiomer excess (i.e., the percentages of different enantiomers). The feasibility of the proposal with chiral molecules confined in hollow-core photonic crystal fiber is also discussed.
Chirality has been extensively studied for well over a century, and its potential applications range from optics to chemistry, medicine, and biology. Ingenious experiments have been designed to measure this naturally small effect. Here we discuss the possibility of producing a medium having a large chiral effect by using the ideas of coherent control. The coherent fields resonant with appropriate transitions in atomic or molecular systems can be used to manipulate the optical properties of a medium. We demonstrate experimentally very large magnetochiral anisotropy by using electromagnetic fields in atomic Rb vapors.
Electromagnetically induced transparency and lasing without inversion are optical manifestations of quantum coherence control. Here we theoretically investigate these effects in a chiral molecule, coherently driven by an optical pump, finding that signal fields can undergo chiroptical absorption quenching or amplification within particular spectral windows at pump intensities as low as ≈ 1kW/cm 2 . Our calculations reveal that molecular chirality has the capacity to dramatically alter quantum coherence phenomena at peculiar wavelength ranges, modulating efficiently circular dichroism depending on the polarisation state of both pump and signal fields and the molecular orientation. We find that, for a given molecular orientation, the dissymmetry factor probed upon right/left-circular polarisation excitation by the signal can get maximised by pump polarisation tuning and the signal direction. By averaging over impinging signal orientations, we find that the orientation-averaged dissymmetry factor can diverge owing to electromagnetically induced transparency producing vanishing averaged absorption cross-sections.