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Pulse shaping for mode-selective ultrafast coherent Raman spectroscopy of highly scattering solids
Dmitry Pestov, Xi Wang, Robert K. Murawski, Gombojav O. Ariunbold, Vladimir A. Sautenkov, and Alexei V. Sokolov »View Author Affiliations
1Institute for Quantum Studies and Department of Physics, Texas A&M University, College Station, Texas 77843, USA
2Current address: Department of Chemistry, Michigan State University, East Lansing, Michigan 48824, USA
3Current address: Department of Physics, Drew University, Madison, New Jersey 07940, USA
4Lebedev Physical Institute of the Russian Academy of Sciences, 53 Leninsky prospect, Moscow 119991, Russia
*Corresponding author: dspestov@gmail.com
JOSA B, Vol. 25, Issue 5, pp. 768-772 (2008)
http://dx.doi.org/10.1364/JOSAB.25.000768
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Abstract
We report on mode-selective ultrafast coherent anti-Stokes Raman spectroscopy (CARS) of a powder of sodium dipicolinate. We produce a pair of stretched laser pulses with precisely adjusted matching chirp rates. We use the pulses for frequency-resolved excitation of coherent molecular vibrations in this highly scattering medium. The induced oscillations are probed with the third delayed ultrashort laser pulse. Since the attained spectral width of the pump-Stokes excitation band is on the order of the spacing between the Raman lines, time-resolved CARS measurements reveal single-mode as well as double-mode coherence decay dynamics, depending on the timing between the pump and Stokes pulses. For a fixed probe pulse delay, the sweeping of the arrival time for one of the preparation pulses maps out the CARS spectrum of the analyte.
© 2008 Optical Society of America
OCIS Codes
(300.6230) Spectroscopy : Spectroscopy, coherent anti-Stokes Raman scattering
(300.6290) Spectroscopy : Spectroscopy, four-wave mixing
(300.6500) Spectroscopy : Spectroscopy, time-resolved
(300.6530) Spectroscopy : Spectroscopy, ultrafast
ToC Category:
Spectroscopy
History
Original Manuscript: December 14, 2007
Manuscript Accepted: February 4, 2008
Published: April 22, 2008
Virtual Issues
Vol. 3, Iss. 6 Virtual Journal for Biomedical Optics
Citation
Dmitry Pestov, Xi Wang, Robert K. Murawski, Gombojav O. Ariunbold, Vladimir A. Sautenkov, and Alexei V. Sokolov, "Pulse shaping for mode-selective ultrafast coherent Raman spectroscopy of highly scattering solids," J. Opt. Soc. Am. B 25, 768-772 (2008)
http://www.opticsinfobase.org/vjbo/abstract.cfm?URI=josab-25-5-768
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References
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- A. S. Weling, B. B. Hu, N. M. Froberg, and D. H. Auston, “Generation of tunable narrow-band Thz radiation from large-aperture photoconducting antennas,” Appl. Phys. Lett. 64, 137-139 (1994). [CrossRef]
- E. Gershgoren, R. A. Bartels, J. T. Fourkas, R. Tobey, M. M. Murnane, and H. C. Kapteyn, “Simplified setup for high-resolution spectroscopy that uses ultrashort pulses,” Opt. Lett. 28, 361-363 (2003). [CrossRef] [PubMed]
- R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002). [CrossRef] [PubMed]
- A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998). [CrossRef] [PubMed]
- A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998). [CrossRef] [PubMed]
- A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998). [CrossRef] [PubMed]
- V. V. Lozovoy, B. I. Grimberg, E. J. Brown, I. Pastirk, and M. Dantus, “Femtosecond spectrally dispersed three-pulse four-wave mixing: the role of sequence and chirp in controlling intramolecular dynamics,” J. Raman Spectrosc. 31, 41-49 (2000). [CrossRef]
- A. V. Sokolov, M. Y. Shverdin, D. R. Walker, D. D. Yavuz, A. M. Burzo, G. Y. Yin, and S. E. Harris, “Generation and control of femtosecond pulses by molecular modulation,” J. Mod. Opt. 52, 285-304 (2005). [CrossRef]
- B. D. Prince, A. Chakraborty, B. M. Prince, and H. U. Stauffer, “Development of simultaneous frequency- and time-resolved coherent anti-Stokes Raman scattering for ultrafast detection of molecular Raman spectra,” J. Chem. Phys. 125, 044502 (2006). [CrossRef]
- A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000). [CrossRef]
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- B. W. Xu, J. M. Gunn, J. M. Dela Cruz, V. V. Lozovoy, and M. Dantus, “Quantitative investigation of the multiphoton intrapulse interference phase scan method for simultaneous phase measurement and compensation of femtosecond laser pulses,” J. Opt. Soc. Am. B 23, 750-759 (2006). [CrossRef]
- V. V. Lozovoy, I. Pastirk, and M. Dantus, “Multiphoton intrapulse interference. IV. Ultrashort laser pulse spectral phase characterization and compensation,” Opt. Lett. 29, 775-777 (2004). [CrossRef] [PubMed]
- V. V. Lozovoy, B. I. Grimberg, E. J. Brown, I. Pastirk, and M. Dantus, “Femtosecond spectrally dispersed three-pulse four-wave mixing: the role of sequence and chirp in controlling intramolecular dynamics,” J. Raman Spectrosc. 31, 41-49 (2000). [CrossRef]
- D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007). [CrossRef] [PubMed]
- D. Oron, N. Dudovich, and Y. Silberberg, “Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy,” Phys. Rev. Lett. 90, 213902 (2003). [CrossRef] [PubMed]
- N. Dudovich, D. Oron, and Y. Silberberg, “Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512-514 (2002). [CrossRef] [PubMed]
- D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Quantum control of coherent anti-Stokes Raman processes,” Phys. Rev. A 65, 043408 (2002). [CrossRef]
- D. Oron, N. Dudovich, D. Yelin, and Y. Silberberg, “Narrow-band coherent anti-Stokes Raman signals from broad-band pulses,” Phys. Rev. Lett. 88, 063004 (2002). [CrossRef] [PubMed]
- T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85, 25-27 (2004). [CrossRef]
- A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000). [CrossRef]
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- A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998). [CrossRef] [PubMed]
- D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005). [CrossRef] [PubMed]
- V. V. Lozovoy, B. I. Grimberg, E. J. Brown, I. Pastirk, and M. Dantus, “Femtosecond spectrally dispersed three-pulse four-wave mixing: the role of sequence and chirp in controlling intramolecular dynamics,” J. Raman Spectrosc. 31, 41-49 (2000). [CrossRef]
- B. D. Church and H. Halvorson, “Dependence of the heat resistance of bacterial endospores on their dipicolinic acid content,” Nature 183, 124-125 (1959). [CrossRef] [PubMed]
- A. V. Sokolov, M. Y. Shverdin, D. R. Walker, D. D. Yavuz, A. M. Burzo, G. Y. Yin, and S. E. Harris, “Generation and control of femtosecond pulses by molecular modulation,” J. Mod. Opt. 52, 285-304 (2005). [CrossRef]
- A. V. Sokolov and S. E. Harris, “Ultrashort pulse generation by molecular modulation,” J. Opt. B: Quantum Semiclassical Opt. 5, R1-R26 (2003). [CrossRef]
- T. Hellerer, A. M. K. Enejder, and A. Zumbusch, “Spectral focusing: high spectral resolution spectroscopy with broad-bandwidth laser pulses,” Appl. Phys. Lett. 85, 25-27 (2004). [CrossRef]
- R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, “Terahertz quantum beats in molecular liquids,” Chem. Phys. Lett. 133, 373-377 (1987). [CrossRef]
- A. S. Weling, B. B. Hu, N. M. Froberg, and D. H. Auston, “Generation of tunable narrow-band Thz radiation from large-aperture photoconducting antennas,” Appl. Phys. Lett. 64, 137-139 (1994). [CrossRef]
- D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007). [CrossRef] [PubMed]
- R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, “Terahertz quantum beats in molecular liquids,” Chem. Phys. Lett. 133, 373-377 (1987). [CrossRef]
- M. C. Zhi, D. Pestov, X. Wang, R. K. Murawski, Y. V. Rostovtsev, Z. E. Sariyanni, V. A. Sautenkov, N. G. Kalugin, and A. V. Sokolov, “Concentration dependence of femtosecond coherent anti-Stokes Raman scattering in the presence of strong absorption,” J. Opt. Soc. Am. B 24, 1181-1186 (2007). [CrossRef]
- D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005). [CrossRef] [PubMed]
- E. Gershgoren, R. A. Bartels, J. T. Fourkas, R. Tobey, M. M. Murnane, and H. C. Kapteyn, “Simplified setup for high-resolution spectroscopy that uses ultrashort pulses,” Opt. Lett. 28, 361-363 (2003). [CrossRef] [PubMed]
- R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002). [CrossRef] [PubMed]
- M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, “FAST CARS: engineering a laser spectroscopic technique for rapid identification of bacterial spores,” Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002). [CrossRef] [PubMed]
- A. Assion, T. Baumert, M. Bergt, T. Brixner, B. Kiefer, V. Seyfried, M. Strehle, and G. Gerber, “Control of chemical reactions by feedback-optimized phase-shaped femtosecond laser pulses,” Science 282, 919-922 (1998). [CrossRef] [PubMed]
- D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005). [CrossRef] [PubMed]
- A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000). [CrossRef]
- D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005). [CrossRef] [PubMed]
- R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002). [CrossRef] [PubMed]
- R. Leonhardt, W. Holzapfel, W. Zinth, and W. Kaiser, “Terahertz quantum beats in molecular liquids,” Chem. Phys. Lett. 133, 373-377 (1987). [CrossRef]
- B. W. Xu, J. M. Gunn, J. M. Dela Cruz, V. V. Lozovoy, and M. Dantus, “Quantitative investigation of the multiphoton intrapulse interference phase scan method for simultaneous phase measurement and compensation of femtosecond laser pulses,” J. Opt. Soc. Am. B 23, 750-759 (2006). [CrossRef]
- V. V. Lozovoy, I. Pastirk, and M. Dantus, “Multiphoton intrapulse interference. IV. Ultrashort laser pulse spectral phase characterization and compensation,” Opt. Lett. 29, 775-777 (2004). [CrossRef] [PubMed]
- V. V. Lozovoy, B. I. Grimberg, E. J. Brown, I. Pastirk, and M. Dantus, “Femtosecond spectrally dispersed three-pulse four-wave mixing: the role of sequence and chirp in controlling intramolecular dynamics,” J. Raman Spectrosc. 31, 41-49 (2000). [CrossRef]
- M. O. Scully, G. W. Kattawar, R. P. Lucht, T. Opatrny, H. Pilloff, A. Rebane, A. V. Sokolov, and M. S. Zubairy, “FAST CARS: engineering a laser spectroscopic technique for rapid identification of bacterial spores,” Proc. Natl. Acad. Sci. U.S.A. 99, 10994-11001 (2002). [CrossRef] [PubMed]
- A. Materny, T. Chen, M. Schmitt, T. Siebert, A. Vierheilig, V. Engel, and W. Kiefer, “Wave packet dynamics in different electronic states investigated by femtosecond time-resolved four-wave-mixing spectroscopy,” Appl. Phys. B 71, 299-317 (2000). [CrossRef]
- D. Meshulach and Y. Silberberg, “Coherent quantum control of multiphoton transitions by shaped ultrashort optical pulses,” Phys. Rev. A 60, 1287-1292 (1999). [CrossRef]
- D. Pestov, M. C. Zhi, Z. E. Sariyanni, N. G. Kalugin, A. A. Kolomenskii, R. Murawski, G. G. Paulus, V. A. Sautenkov, H. Schuessler, A. V. Sokolov, G. R. Welch, Y. V. Rostovtsev, T. Siebert, D. A. Akimov, S. Graefe, W. Kiefer, and M. O. Scully, “Visible and UV coherent Raman spectroscopy of dipicolinic acid,” Proc. Natl. Acad. Sci. U.S.A. 102, 14976-14981 (2005). [CrossRef] [PubMed]
- M. C. Zhi, D. Pestov, X. Wang, R. K. Murawski, Y. V. Rostovtsev, Z. E. Sariyanni, V. A. Sautenkov, N. G. Kalugin, and A. V. Sokolov, “Concentration dependence of femtosecond coherent anti-Stokes Raman scattering in the presence of strong absorption,” J. Opt. Soc. Am. B 24, 1181-1186 (2007). [CrossRef]
- D. Pestov, R. K. Murawski, G. O. Ariunbold, X. Wang, M. C. Zhi, A. V. Sokolov, V. A. Sautenkov, Y. V. Rostovtsev, A. Dogariu, Y. Huang, and M. O. Scully, “Optimizing the laser-pulse configuration for coherent Raman spectroscopy,” Science 316, 265-268 (2007). [CrossRef] [PubMed]
- E. Gershgoren, R. A. Bartels, J. T. Fourkas, R. Tobey, M. M. Murnane, and H. C. Kapteyn, “Simplified setup for high-resolution spectroscopy that uses ultrashort pulses,” Opt. Lett. 28, 361-363 (2003). [CrossRef] [PubMed]
- R. A. Bartels, T. C. Weinacht, S. R. Leone, H. C. Kapteyn, and M. M. Murnane, “Nonresonant control of multimode molecular wave packets at room temperature,” Phys. Rev. Lett. 88, 033001 (2002). [CrossRef] [PubMed]
- A. M. Zheltikov and A. N. Naumov, “High-resolution four-photon spectroscopy with chirped pulses,” Quantum Electron. 30, 606-610 (2000). [CrossRef]
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