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Frontiers in Optics

Applications of Molecular Coherence

Alexei V. Sokolov

Published Jan 1, 2008• 0 citations
Publisher

Abstract

I will review the developments that have resulted in extending the ideas of atomic coherence to molecular physics. Macroscopic molecular coherence allows broadband collinear generation of Raman sidebands, opening possibilities for compression of optical sub-cycle pulses, and for non-sinusoidal field synthesis; increased coherence also enables improvements in optical detection and sensing applications.

DOI
10.1364/fio.2008.swd1

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I will review the developments that have resulted in extending the ideas of atomic coherence to molecular physics. Macroscopic molecular coherence allows broadband collinear generation of Raman sidebands, opening possibilities for compression of optical sub-cycle pulses, and for non-sinusoidal field synthesis; increased coherence also enables improvements in optical detection and sensing applications.
Recent experiments have shown that coherent molecular oscillations may generate a comb of coherent collinear sidebands with 50,000 cm/sup -1/ of spectral bandwidth. The essence of this technique is the use of a Raman transition with a sufficiently large coherence that the generation and phase slip length are of the same order. The coherence is established by driving the molecular transition with two single-mode laser fields slightly detuned from the Raman resonance, so as to excite a single molecular superposition state. This talk will summarize the characteristics of this light source and describe two recent experiments which show the mutual coherence of the generated sidebands.
We have demonstrated that coherent molecular modulation can result in the collinear generation of mutually-coherent spectral sidebands that extend in frequency from the infrared to the far ultraviolet. Our technique is based on adiabatic preparation of a highly coherent molecular superposition-state, which is achieved by using narrow-linewidth lasers slightly detuned from a Raman resonance. The phases of the resultant Stokes and anti-Stokes sidebands are adjusted in order to synthesize desired single-cycle pulse trains at the target. In this article we review recent improvements and developments in this area, including: techniques for increasing the number of generated sidebands; synchronization of the pulse trains with the molecular motion in the given molecular system; laser self-focusing and spatial soliton formation due to the coherent interaction of light with oscillating molecules. In the future, this Raman source may produce sub-cycle optical pulses, and allow synthesis of waveforms where the electric field is a predetermined function of time, not limited to a quasi-sinusoidal oscillation.
We use molecular deuterium and two driving lasers to demonstrate collinear generation of mutually coherent equidistant sidebands, covering $50000{\mathrm{cm}}^{\ensuremath{-}1}$ of spectral bandwidth and ranging from $2.94\ensuremath{\mu}\mathrm{m}$ to 195 nm in wavelength. The essential idea is the adiabatic preparation of a single, highly coherent ( $|{\ensuremath{\rho}}_{\mathrm{ab}}|\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0.33$) molecular eigenstate.
Detection and sensing of molecules via their interaction with light opens opportunities for studies ranging from nanoscale single-molecule readout to long-range experiments. Plasmonic antennas allow localized electromagnetic enhancement, allowing Raman-spectroscopic sensing with sub-nanometer spatial resolution. Further signal enhancement can be obtained through the use of molecular coherence - produced either through coherent Raman excitation or via direct infrared driving. The next level of improvements in signal-to-noise ratio will come with the use of properly engineered non-classical states of light.
It is well known that the optical properties of multi-level atomic and molecular system can be controlled and manipulated efficiently using quantum coherence and interference, which has led to many new effects in quantum optics for e.g. lasing action without population inversion, ultraslow light, high resolution nonlinear spectroscopy etc. Recent experimental and theoretical studies have also provided support for the hypothesis that biological systems uses quantum coherence. Nearly perfect excitation energy transfer in photosynthesis is an excellent example of this.\n\nIn this dissertation we studied quantum coherence and interference effects in the transient and the continuous-wave regimes. This study led to (i) the first experimental demonstration of carrier-envelope phase effects on bound-bound atomic excitation in multi-cycle regime (~15 cycles), (ii) a unique possibility for standoff detection of trace gases using their rotational and vibrational spectroscopic signals and from herein called Coherent Raman Umklappscattering, (iii) several possibilities for frequency up-conversion and generation of short-wavelength radiation using quantum coherence (iv) the measurement of spontaneous emission noise intensity in Yoked-superfluorescence scheme.\n\nApplications of the obtained results are development of XUV (X-Ray) lasers, con- trolled superfluorescent (superradiant) emission, carrier-envelope phase effects, coherent Raman scattering in the backward direction, enhancement of efficiency for generating radiation in XUV and X-Ray regime using quantum coherence with and without population inversion and to extend XUV and X-Ray lasing to ~4.023 nm in Helium-like carbon.