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Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy


Molecular vibrations have oscillation periods that reflect the molecular structure, and are hence being used as a spectroscopic fingerprint for detection and identification. At present, all nonlinear spectroscopy schemes use two or more laser beams to measure such vibrations1. The availability of ultrashort (femtosecond) optical pulses with durations shorter than typical molecular vibration periods has enabled the coherent excitation of molecular vibrations using a single pulse2. Here we perform single-pulse vibrational spectroscopy on several molecules in the liquid phase, where both the excitation and the readout processes are performed by the same pulse. The main difficulty with single-pulse spectroscopy is that all vibrational levels with energies within the pulse bandwidth are excited. We achieve high spectral resolution, nearly two orders of magnitude better than the pulse bandwidth, by using quantum coherent control techniques. By appropriately modulating the spectral phase of the pulse we are able to exploit the quantum interference between multiple paths to selectively populate a given vibrational level, and to probe this population using the same pulse. This scheme, using a single broadband laser source, is particularly attractive for nonlinear microscopy applications, as we demonstrate by constructing a coherent anti-Stokes Raman (CARS) microscope operating with a single laser beam.

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Figure 1: Graphic description of the coherent anti-Stokes Raman (CARS) process and the experimental set-up.
Figure 2: Single-pulse CARS spectroscopy of various organic molecules in the liquid phase.
Figure 3: Demonstration of the nonresonant background suppression.
Figure 4: Depth-resolved single-pulse CARS images of a glass capillary plate with 10-µm holes filled with CH2Br2 (resonant at 577 cm-1).


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We thank D. Mandelik for his aid in preparing the microscope samples. Financial support by the Israeli Science Foundation and by the Bundesministerium fur Bildung und Forschung is gratefully acknowledged.

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Correspondence to Yaron Silberberg.

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Dudovich, N., Oron, D. & Silberberg, Y. Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy. Nature 418, 512–514 (2002).

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