Abstract

We use experimental search space mapping to examine the problem of selective nonlinear excitation with binary phase shaped femtosecond laser pulses. The search space maps represent a graphical view of all the possible solutions to the selective nonlinear excitation problem along with their experimental degrees of success. Using the information learned from these maps, we generate narrow lines with low background in second harmonic generation and stimulated Raman scattering spectra.

© 2005 Optical Society of America

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References

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  1. A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, "Femtosecond pulse sequences used for optical manipulation of molecular-motion," Science 247, 1317-1319 (1990).
    [CrossRef] [PubMed]
  2. Z. Zheng, and A. M. Weiner, "Coherent control of second harmonic generation using spectrally phase coded femtosecond waveforms," Chem. Phys. 267, 161-171 (2001).
    [CrossRef]
  3. D. Meshulach, and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature 396, 239-242 (1998).
    [CrossRef]
  4. 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]
  5. J. M. Dela Cruz, I. Pastirk, V. V. Lozovoy, K. A. Walowicz, and M. Dantus, "Multiphoton intrapulse interference 3: Probing microscopic chemical environments," J. Phys. Chem. A 108, 53-58 (2004).
    [CrossRef]
  6. H. A. Rabitz, M. M. Hsieh, and C. M. Rosenthal, "Quantum optimally controlled transition landscapes," Science 303, 1998-2001 (2004).
    [CrossRef] [PubMed]
  7. K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, "Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases," J. Phys. Chem. A 106, 9369-9373 (2002).
    [CrossRef]
  8. V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, "Multiphoton intrapulse interference. II Control of two- and three-photon laser induced fluorescence with shaped pulses," J. Chem. Phys. 118, 3187-3196 (2003).
    [CrossRef]
  9. I. Pastirk, J. M. Dela Cruz, K. A. Walowicz, V. V. Lozovoy, and M. Dantus, "Selective two-photon microscopy with shaped femtosecond pulses," Opt. Express 11, 1695-1701 (2003)<a href= http://www.opticsexpress.org/abstract.cfm?URI=OPEX-11-14-1695>http://www.opticsexpress.org/abstract.cfm?URI=OPEX-11-14-1695</a>.
    [CrossRef] [PubMed]
  10. V. V. Lozovoy, and M. Dantus, "Systematic control of nonlinear optical processes using optimally shaped femtosecond pulses," Chem. Phys. Chem. 6, 1952-1967 (2005).
    [CrossRef]
  11. A. M. Weiner, "Femtosecond pulse shaping using spatial light modulators," Rev. Sci. Instrum. 71, 1929-1960 (2000).
    [CrossRef]
  12. 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]
  13. B. Xu, J. M. Gunn, J. M. DelaCruz, V. V. Lozovoy, and M. Dantus, "Quantitative investigation of the MIIPS method for phase measurement and compensation of femtosecond laser pulses," J.Opt. Soc. Am. B, in press.
  14. V. V. Lozovoy, B. Xu, J. C. Shane, and M. Dantus, "Selective nonlinear excitation with pseudorandom Galois fields," to be published (2005).
  15. J. M. Dela Cruz, I. Pastirk, M. Comstock, V. V. Lozovoy, and M. Dantus, "Use of coherent control methods through scattering biological tissue to achieve functional imaging," P. Natl. Acad. Sci. USA 101, 16996-17001 (2004).
    [CrossRef]
  16. I. Pastirk, M. Kangas, and M. Dantus, "Multidimensional analytical method based on binary phase shaping of femtosecond pulses," J. Phys. Chem. A 109, 2413-2416 (2005).
    [CrossRef]
  17. J. M. Dela Cruz, V. V. Lozovoy, and M. Dantus, "Quantitative mass spectrometric identification of isomers applying coherent laser control," J. Phys. Chem. A 109, 8447-8450 (2005).
    [CrossRef]

Chem. Phys. (1)

Z. Zheng, and A. M. Weiner, "Coherent control of second harmonic generation using spectrally phase coded femtosecond waveforms," Chem. Phys. 267, 161-171 (2001).
[CrossRef]

Chem. Phys. Chem. (1)

V. V. Lozovoy, and M. Dantus, "Systematic control of nonlinear optical processes using optimally shaped femtosecond pulses," Chem. Phys. Chem. 6, 1952-1967 (2005).
[CrossRef]

J. Chem. Phys. (1)

V. V. Lozovoy, I. Pastirk, K. A. Walowicz, and M. Dantus, "Multiphoton intrapulse interference. II Control of two- and three-photon laser induced fluorescence with shaped pulses," J. Chem. Phys. 118, 3187-3196 (2003).
[CrossRef]

J. Phys. Chem. A (4)

K. A. Walowicz, I. Pastirk, V. V. Lozovoy, and M. Dantus, "Multiphoton intrapulse interference. 1. Control of multiphoton processes in condensed phases," J. Phys. Chem. A 106, 9369-9373 (2002).
[CrossRef]

J. M. Dela Cruz, I. Pastirk, V. V. Lozovoy, K. A. Walowicz, and M. Dantus, "Multiphoton intrapulse interference 3: Probing microscopic chemical environments," J. Phys. Chem. A 108, 53-58 (2004).
[CrossRef]

I. Pastirk, M. Kangas, and M. Dantus, "Multidimensional analytical method based on binary phase shaping of femtosecond pulses," J. Phys. Chem. A 109, 2413-2416 (2005).
[CrossRef]

J. M. Dela Cruz, V. V. Lozovoy, and M. Dantus, "Quantitative mass spectrometric identification of isomers applying coherent laser control," J. Phys. Chem. A 109, 8447-8450 (2005).
[CrossRef]

J.Opt. Soc. Am. B (1)

B. Xu, J. M. Gunn, J. M. DelaCruz, V. V. Lozovoy, and M. Dantus, "Quantitative investigation of the MIIPS method for phase measurement and compensation of femtosecond laser pulses," J.Opt. Soc. Am. B, in press.

Nature (1)

D. Meshulach, and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature 396, 239-242 (1998).
[CrossRef]

Opt. Express (1)

Opt. Lett. (1)

P. Natl. Acad. Sci. (1)

J. M. Dela Cruz, I. Pastirk, M. Comstock, V. V. Lozovoy, and M. Dantus, "Use of coherent control methods through scattering biological tissue to achieve functional imaging," P. Natl. Acad. Sci. USA 101, 16996-17001 (2004).
[CrossRef]

Phys. Rev. Lett. (1)

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]

Rev. Sci. Instrum. (1)

A. M. Weiner, "Femtosecond pulse shaping using spatial light modulators," Rev. Sci. Instrum. 71, 1929-1960 (2000).
[CrossRef]

Science (2)

H. A. Rabitz, M. M. Hsieh, and C. M. Rosenthal, "Quantum optimally controlled transition landscapes," Science 303, 1998-2001 (2004).
[CrossRef] [PubMed]

A. M. Weiner, D. E. Leaird, G. P. Wiederrecht, and K. A. Nelson, "Femtosecond pulse sequences used for optical manipulation of molecular-motion," Science 247, 1317-1319 (1990).
[CrossRef] [PubMed]

Other (1)

V. V. Lozovoy, B. Xu, J. C. Shane, and M. Dantus, "Selective nonlinear excitation with pseudorandom Galois fields," to be published (2005).

Supplementary Material (4)

» Media 1: GIF (896 KB)     
» Media 2: GIF (714 KB)     
» Media 3: AVI (809 KB)     
» Media 4: AVI (446 KB)     

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Figures (3)

Fig. 1.
Fig. 1.

Nonlinear spectra of phase modulated pulses. The dashed line is the spectrum of a Gaussian transform-limited (flat spectral phase) pulse. (a) Maximization or minimization of nonlinear spectra at a selected frequency. (b) Generation of a narrow peak at a selected frequency with low background (the goal of this project).

Fig. 2.
Fig. 2.

Experimental mapping of selective SHG (left) and SRS (right) at the center of the spectrum (see Fig. 1(b). X and y coordinates are the decimal representations of the left and right halves of the binary phase sequences, respectively, and color as z coordinate is the experimentally measured signal to background ratio of nonlinear excitation. Here, phase sequences with high S/B ratios are shown in red, while sequences with low S/B ratios are shown in black. Arrows point to the locations of the global maxima. [Media 1] [Media 2]

Fig. 3.
Fig. 3.

Experimental generation (dots) and simulation (red) of narrow-band and low-background nonlinear fields using optimized binary phase functions. (a) and (b) Phase (black) and amplitude (red) modulation was imprinted with the SLM on a broad fundamental pulse. (c) SHG spectrum measured with a nonlinear crystal. (d) SRS spectrum recorded as the Fourier transform of the autocorrelation trace using a collinear Michelson interferometer. [Media 3] [Media 4]

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