Abstract

In most coherent control experiments with femtosecond pulses, the temporal shape of the pulses is maintained throughout the interaction region. Here we show how pulses can be controlled such that their shapes vary rapidly even when propagating very short distances of a few micrometers. This changing pulse shape has a significant effect on coherent nonlinear optical processes. Here we study third-harmonic generation induced by a coherently controlled excitation pulse whose temporal profile changes along the axial coordinate. We show how such manipulations can be used to improve the axial resolution in a multiphoton optical microscope.

© 2005 Optical Society of America

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References

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Appl. Phys. Lett. (1)

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, ”Nonlinear scanning laser microscopy by third harmonic generation,” Appl. Phys. Lett. 70, 922 (1997).
[CrossRef]

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

D. Oron, Y. Silberberg, ”Harmonic generation with temporally focused ultrashort pulses,” Accepted for publication in J. Opt. Soc. Am. B (2005).
[CrossRef]

Nature (2)

N. Dudovich, D. Oron, Y. Silberberg, ”Single-pulse coherently-controlled nonlinear Raman spectroscopy and microscopy,” Nature 418, 512 (2002).
[CrossRef] [PubMed]

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

Opt. Express (2)

Opt. Lett. (5)

Science (3)

P. Tian, D. Keusters, Y. Suzaki, W.S. Warren, ”Femtosecond phase-coherent two dimensional spectroscopy,” Science 300, 1553 (2003).
[CrossRef] [PubMed]

T. Feurer, J.C. Vaughan, K.A. Nelson, ”Spatiotemporal coherent control of lattice vibrational waves,” Science, 299, 374 (2003).
[CrossRef] [PubMed]

A. Assion et al., ”Control of chemical reactions by feedback-optimized pulse-shaped femtosecond laser pulses,” Science 282, 919 (1998).
[CrossRef] [PubMed]

Other (1)

R. Boyd, Nonlinear Optics, (Academic press, New York, 1992).

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Figures (5)

Fig. 1.
Fig. 1.

Experimental setup of our coherent control apparatus: The input beam impinges upon a grating, aligned perpendicular to the optic axis of a high magnification telescope, comprised of an cylindrical lens and the microscope objective (with focal lengths f 1and f 2, respectively). A phase-and-polarization SLM is placed at the Fourier plane, next to the microscope objective. The sample is mounted on a piezoelectric stage. The integrated THG signal is collected in the forward direction, filtered, and measured by a photomultiplier tube.

Fig. 2.
Fig. 2.

Enhancement of the cross-sectioning capability by phase-only control: Plotted are the measured Z-scans with either no phase applied to the SLM (solid blue line) And with a π phase step applied at the center frequency of the pulse (dashed red line). The difference between the two (dashdotted green line) exhibits better cross-sectioning and complete rejection of the response at the tails.

Fig. 3.
Fig. 3.

The effect of dispersion on an unshaped pulse (a) and on the π step pulse (b). Shown are the temporal profiles of the pulses at z=0 (solid blue lines) and at the FWHM of the THG response (dashed green lines). As can be seen, dispersion reduces the THG yield for unshaped pulses but increases the THG yield from the π step pulse regardless of its sign.

Fig. 4.
Fig. 4.

Control of THG by modification of the transient polarization at the temporal focal plane: THG signal as a function of the relative phase applied to the vertically polarized and horizontally polarized components of the excitation pulse without a polarizer (solid black line), with a polarizer at 45° (dashdotted red line) and with a polarizer at -45° (dashed blue line).

Fig. 5.
Fig. 5.

Enhancement of the cross-sectioning capability by phase-and-polarization control: Plotted are the measured Z-scans with either a π relative phase between the vertical and the horizontal polarizations (solid blue line) or a π/2 relative phase (dashed red line). The difference between the two (dashdotted green line) exhibits better cross-sectioning than observed in Fig. 2.

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