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Recent advances in coherent Raman spectroscopy hold exciting promise for many potential applications. For example, a technique, mitigating the nonresonant four-wave-mixing noise while maximizing the Raman-resonant signal, has been developed and applied to the problem of real-time detection of bacterial endospores. After a brief review of the technique essentials, we show how extensions of our earlier experimental work [Pestov D, et al. (2007) Science 316:265-268] yield single-shot identification of a small sample of Bacillus subtilis endospores ([approximately equal to] [10.sup.4] spores). The results convey the utility of the technique and its potential for 'on-the-fly' detection of biohazards, such as Bacillus anthracis. The application of optimized coherent anti-Stokes Raman scattering scheme to problems requiring chemical specificity and short signal acquisition times is demonstrated.

We use time-resolved coherent Raman spectroscopy to obtain molecule-specific signals from dipicolinic acid (DPA), which is a marker molecule for bacterial spores. We use femtosecond laser pulses in both visible and UV spectral regions and compare experimental results with theoretical predictions. By exciting vibrational coherence on more than one mode simultaneously, we observe a quantum beat signal that can be used to extract the parameters of molecular motion in DPA. The signal is enhanced when an UV probe pulse is used, because its frequency is near-resonant to the first excited electronic state of the molecule. The capability for unambiguous identification of DPA molecules will lead to a technique for real-time detection of spores. molecular spectroscopy | coherent anti-Stokes Raman scattering | bacterial spores | molecular coherence | nonlinear optics

We have studied coherent emission from ambient air and demonstrated efficient generation of laser-like beams directed both forward and backward with respect to a nanosecond ultraviolet pumping laser beam. The generated optical gain is a result of two-photon photolysis of atmospheric O2, followed by two-photon excitation of atomic oxygen. We have analyzed the temporal shapes of the emitted pulses and have observed very short duration intensity spikes as well as a large Rabi frequency that corresponds to the emitted field. Our results suggest that the emission process exhibits nonadiabatic atomic coherence, which is similar in nature to Dicke superradiance where atomic coherence is large and can be contrasted with ordinary lasing where atomic coherence is negligible. This atomic coherence in oxygen adds insight to the optical emission physics and holds promise for remote sensing techniques employing nonlinear spectroscopy. [ABSTRACT FROM AUTHOR]