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Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb


The control of the broadband frequency comb1 emitted from a mode-locked femtosecond laser has permitted a wide range of scientific and technological advances—ranging from the counting of optical cycles for next-generation atomic clocks1,2 to measurements of phase-sensitive high-field processes3. A unique advantage of the stabilized frequency comb is that it provides, in a single laser beam, about a million optical modes with very narrow linewidths4 and absolute frequency positions known to better than one part in 1015 (ref. 5). One important application of this vast array of highly coherent optical fields is precision spectroscopy, in which a large number of modes can be used to map internal atomic energy structure and dynamics6,7. However, an efficient means of simultaneously identifying, addressing and measuring the amplitude or relative phase of individual modes has not existed. Here we use a high-resolution disperser8,9 to separate the individual modes of a stabilized frequency comb into a two-dimensional array in the image plane of the spectrometer. We illustrate the power of this technique for high-resolution spectral fingerprinting of molecular iodine vapour, acquiring in a few milliseconds absorption images covering over 6 THz of bandwidth with high frequency resolution. Our technique for direct and parallel accessing of stabilized frequency comb modes could find application in high-bandwidth spread-spectrum communications with increased security, high-resolution coherent quantum control, and arbitrary optical waveform synthesis10 with control at the optical radian level.

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Figure 1: Experimental set-up.
Figure 2: Two-dimensional spectrograms of optical frequency ‘brush’.
Figure 3: Concatenated line spectra.
Figure 4: Absorption spectra of P(32)6–3, R(59)8–4 and R(53)8–4 transitions in iodine.


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We thank A. M. Weiner for discussions about the VIPA spectrometer, and J. Ye for discussions that motivated our application of frequency combs to broadband spectroscopy. We further thank J. Stalnaker and Y. LeCoq for their comments on this manuscript, and H. Kato for the CW iodine spectroscopy data. This paper is a contribution of the National Institute of Standards and Technology, with partial support from DARPA.

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Correspondence to Scott A. Diddams.

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Diddams, S., Hollberg, L. & Mbele, V. Molecular fingerprinting with the resolved modes of a femtosecond laser frequency comb. Nature 445, 627–630 (2007).

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