Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy

Abstract

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.

Your institute does not have access to this article

Relevant articles

Open Access articles citing this article.

Access options

Buy article

Get time limited or full article access on ReadCube.

$32.00

All prices are NET prices.

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).

References

  1. Kiefer, W. in Infrared and Raman Spectroscopy (ed. Schrader, B.) 162–188 (VCH, Weinheim, 1995)

  2. Yan, Y. X., Cheng, L. T. & Nelson, K. A. in Advances in Spectroscopy (eds Clark, R. J. H. & Hester, R. E.) Vol. 16, 299–355 (Wiley, Chichester, 1988)

    Google Scholar 

  3. Levenson, M. D. Introduction to Nonlinear Laser Spectroscopy (Academic, New York, 1982)

    Google Scholar 

  4. Leonhardt, R., Holzapfel, W., Zinth, W. & Kaiser, W. Terahertz quantum beats in molecular liquids. Chem. Phys. Lett. 133, 373–377 (1986)

    ADS  Article  Google Scholar 

  5. Cheng, J., Volkmer, A., Book, L. D. & Xie, X. S. An epi-detected coherent anti-Stokes Raman scattering (E-CARS) microscope with high spectral resolution and high sensitivity. J. Phys. Chem. B 105, 1277–1280 (2001)

    CAS  Article  Google Scholar 

  6. Tannor, D. J. & Rice, S. A. Control of selectivity of chemical reaction via control of wavepacket evolution. J. Chem. Phys. 83, 5013–5018 (1985)

    ADS  CAS  Article  Google Scholar 

  7. Shapiro, M. & Brumer, P. Laser control of product quantum state populations in unimolecular reactions. J. Chem. Phys. 84, 4103–4104 (1986)

    ADS  CAS  Article  Google Scholar 

  8. Warren, W. S., Rabitz, H. & Dahleh, M. Coherent control of quantum dynamics: the dream is alive. Science 259, 1581–1589 (1993)

    ADS  MathSciNet  CAS  Article  Google Scholar 

  9. Weiner, A. M., Leaird, D. E., Wiederrecht, G. P. & Nelson, K. A. Femtosecond pulse sequences used for optical manipulation of molecular motion. Science 247, 1317–1319 (1990)

    ADS  CAS  Article  Google Scholar 

  10. Meshulach, D. & Silberberg, Y. Coherent quantum control of two-photon transitions by a femtosecond laser pulse. Nature 396, 239–242 (1998)

    ADS  CAS  Article  Google Scholar 

  11. Judson, S. R. & Rabitz, H. Teaching lasers to control molecules. Phys. Rev. Lett. 68, 1500–1503 (1992)

    ADS  CAS  Article  Google Scholar 

  12. Assion, A. et al. Control of chemical reaction by feedback-optimized phase-shaped femtosecond laser pulses. Science 282, 919–922 (1998)

    ADS  CAS  Article  Google Scholar 

  13. Bartels, R. et al. Shaped pulse optimization of coherent emission of high-harmonic soft X-rays. Nature 406, 164–166 (2000)

    ADS  CAS  Article  Google Scholar 

  14. Weinacht, T. C., Ahn, J. & Bucksbaum, P. H. Controlling the shape of a quantum wavefunction. Nature 397, 233–235 (1999)

    ADS  CAS  Article  Google Scholar 

  15. Oron, D., Dudovich, N., Yelin, D. & Silberberg, Y. Quantum control of coherent anti-Stokes Raman processes. Phys. Rev. A 65, 043408-1–043408-4 (2002)

    ADS  Article  Google Scholar 

  16. Oron, D., Dudovich, N., Yelin, D. & Silberberg, Y. Narrow band coherent anti-Stokes Raman signals from broadband pulses. Phys. Rev. Lett. 88, 063004-1–063004-4 (2002)

    ADS  Article  Google Scholar 

  17. Weiner, A. M. Femtosecond pulse shaping using spatial light modulators. Rev. Sci. Instrum. 71, 1929–1960 (2000)

    ADS  CAS  Article  Google Scholar 

  18. Denk, W., Strickler, J. H. & Webb, W. W. Two-photon laser scanning fluorescence microscopy. Science 248, 73–76 (1990)

    ADS  CAS  Article  Google Scholar 

  19. Barad, Y., Eisenberg, H., Horowitz, M. & Silberberg, Y. Nonlinear scanning laser microscopy by third harmonic generation. Appl. Phys. Lett. 70, 922–924 (1997)

    ADS  CAS  Article  Google Scholar 

  20. Muller, M., Squier, J., Wilson, K. R. & Brakenhoff, G. J. 3D microscopy of transparent objects using third harmonic generation. J. Microsc. 191, 266–274 (1998)

    CAS  Article  Google Scholar 

  21. Zumbusch, A., Holtom, G. R. & Xie, X. S. Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering. Phys. Rev. Lett. 82, 4142–4145 (1999)

    ADS  CAS  Article  Google Scholar 

  22. Potma, E. O., de Boeij, W. P., van Haastert, P. J. M. & Wiersma, D. A. Real-time visualization of intracellular hydrodynamics in single living cells. Proc. Natl Acad. Sci. USA 98, 1577–1582 (2001)

    ADS  CAS  Article  Google Scholar 

  23. Muller, M., Squier, J., de Lange, C. A. & Brakenhoff, G. J. CARS microscopy with folded BoxCARS phasematching. J. Microsc. 197, 150–158 (2000)

    Article  Google Scholar 

Download references

Acknowledgements

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.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Yaron Silberberg.

Ethics declarations

Competing interests

The authors declare that they have no competing financial interests.

Rights and permissions

Reprints and Permissions

About this article

Cite this article

Dudovich, N., Oron, D. & Silberberg, Y. Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy. Nature 418, 512–514 (2002). https://doi.org/10.1038/nature00933

Download citation

  • Received:

  • Accepted:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nature00933

Further reading

Comments

By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing