Abstract

We demonstrate that the intensity of the second harmonic (SH) generated in KTiOPO4 nanoparticles excited with femtosecond laser pulses increases with decreasing duration of the infrared pump pulses. The SH intensity scales, approximately, as the inverse of the laser pulse duration ranging between 13 fs and 200 fs. The SH intensity enhancement requires careful compensation of the high-order spectral phase, being achieved with a genetic algorithm. Using ultrashort laser pulses improves the signal-to-noise ratio and will allow the detection of 10-nm size particles. Finally, we demonstrate that the spectrum of broadband (100 nm) pulses can be shaped to generate non-degenerate sum-frequency mixing. This opens up access to the polarization degrees of freedom of this second-order nonlinear process at the nanoscale.

© 2009 Optical Society of America

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2008 (3)

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

P. Xi, Y. Andegeko, L. R. Weisel, V. V. Lozovoy, and M. Dantus, "Greater Signal and Less Photobleaching in Two-Photon Microscopy with Ultrabroad Bandwidth Femtosecond Pulses," Opt. Commun. 281, 1841-1849 (2008).
[CrossRef]

J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Glez, and J. -P. Wolf, "Nano-FROG: Frequency resolved optical gating by a nanometric object," Opt. Express 16, 10405-10411 (2008), http://www.opticsinfobase.org/abstract.cfm?URI=oe-16-14-10405.
[CrossRef] [PubMed]

2007 (6)

P. Wnuk and C. Radzewicz, "Coherent control and dark pulses in second harmonic generation," Opt. Commun. 272, 496-502 (2007).
[CrossRef]

N. Sandeau, L. Le Xuan, C. Zhou, D. Chauvat, J. -F. Roch, and S. Brasselet, "Defocused imaging of second harmonic generation from a single nanocrystal," Opt. Express 15, 16051-16060 (2007), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-15-24-16051.
[CrossRef] [PubMed]

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

2006 (1)

T. Brixner, F. J. García de Abajo, C. Spindler, and W. Pfeiffer, "Adaptive ultrafast nano-optics in a tight focus," Appl. Phys. B 84, 89-95 (2006).
[CrossRef]

2004 (1)

2003 (1)

W. R. Zipfel, R. M. Williams, and W. W. Webb, "Nonlinear magic: multiphoton microscopy in the biosciences," Nature Biotechnol. 21, 1369-1377 (2003).
[CrossRef]

2002 (1)

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

2001 (1)

2000 (1)

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

1998 (1)

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

1997 (2)

T. Baumert, T. Brixner, V. Seyfried, M. Strehle, and G. Gerber, "Femtosecond pulse shaping by an evolutionary algorithm with feedback," Appl. Phys. B 65, 779-782 (1997).
[CrossRef]

J. B. Guild, C. Xu, and W. W. Webb, "Measurement of group delay dispersion of high numerical aperture objective lenses using two-photon excited fluorescence," Appl. Opt. 36, 397-401 (1997).
[CrossRef] [PubMed]

1993 (1)

W. S. Warren, R. Rabitz, and M. Daleh, "Coherent Control of Quantum Dynamics: The Dream Is Alive," Science 259, 1581-1589 (1993).
[CrossRef] [PubMed]

1992 (1)

B. Broers, L. D. Noordam, and H. B. van Lindenvan den Heuvall, "Diffraction and focusing of spectral energy in multiphoton processes," Phys. Rev. A 46, 2749-2756 (1992).
[CrossRef] [PubMed]

1968 (1)

S. Kurtz and T. Perry, "A powder technique for the evaluation of nonlinear optical materials," IEEE J. Quantum Electron. 4, 333-333 (1968).
[CrossRef]

Aeschlimann, M.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

Andegeko, Y.

P. Xi, Y. Andegeko, L. R. Weisel, V. V. Lozovoy, and M. Dantus, "Greater Signal and Less Photobleaching in Two-Photon Microscopy with Ultrabroad Bandwidth Femtosecond Pulses," Opt. Commun. 281, 1841-1849 (2008).
[CrossRef]

Bauer, M.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

Baumert, T.

T. Baumert, T. Brixner, V. Seyfried, M. Strehle, and G. Gerber, "Femtosecond pulse shaping by an evolutionary algorithm with feedback," Appl. Phys. B 65, 779-782 (1997).
[CrossRef]

Bonacina, L.

J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Glez, and J. -P. Wolf, "Nano-FROG: Frequency resolved optical gating by a nanometric object," Opt. Express 16, 10405-10411 (2008), http://www.opticsinfobase.org/abstract.cfm?URI=oe-16-14-10405.
[CrossRef] [PubMed]

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Boutou, V.

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Brasselet, S.

Brixner, T.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

T. Brixner, F. J. García de Abajo, C. Spindler, and W. Pfeiffer, "Adaptive ultrafast nano-optics in a tight focus," Appl. Phys. B 84, 89-95 (2006).
[CrossRef]

T. Brixner and G. Gerber, "Femtosecond polarization pulse shaping," Opt. Lett.  26, 557-559 (2001).
[CrossRef]

T. Baumert, T. Brixner, V. Seyfried, M. Strehle, and G. Gerber, "Femtosecond pulse shaping by an evolutionary algorithm with feedback," Appl. Phys. B 65, 779-782 (1997).
[CrossRef]

Broers, B.

B. Broers, L. D. Noordam, and H. B. van Lindenvan den Heuvall, "Diffraction and focusing of spectral energy in multiphoton processes," Phys. Rev. A 46, 2749-2756 (1992).
[CrossRef] [PubMed]

Byer, D.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

Chang, C. -H.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Chauvat, D.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

N. Sandeau, L. Le Xuan, C. Zhou, D. Chauvat, J. -F. Roch, and S. Brasselet, "Defocused imaging of second harmonic generation from a single nanocrystal," Opt. Express 15, 16051-16060 (2007), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-15-24-16051.
[CrossRef] [PubMed]

Chen, L. -J.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Chu, S. -W.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Courvoisier, F.

J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Glez, and J. -P. Wolf, "Nano-FROG: Frequency resolved optical gating by a nanometric object," Opt. Express 16, 10405-10411 (2008), http://www.opticsinfobase.org/abstract.cfm?URI=oe-16-14-10405.
[CrossRef] [PubMed]

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Daleh, M.

W. S. Warren, R. Rabitz, and M. Daleh, "Coherent Control of Quantum Dynamics: The Dream Is Alive," Science 259, 1581-1589 (1993).
[CrossRef] [PubMed]

Dantus, M.

P. Xi, Y. Andegeko, L. R. Weisel, V. V. Lozovoy, and M. Dantus, "Greater Signal and Less Photobleaching in Two-Photon Microscopy with Ultrabroad Bandwidth Femtosecond Pulses," Opt. Commun. 281, 1841-1849 (2008).
[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]

Dudovich, N.

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

Extermann, J.

J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Glez, and J. -P. Wolf, "Nano-FROG: Frequency resolved optical gating by a nanometric object," Opt. Express 16, 10405-10411 (2008), http://www.opticsinfobase.org/abstract.cfm?URI=oe-16-14-10405.
[CrossRef] [PubMed]

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Gacoin, T.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

Galez, C.

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

García de Abajo, F. J.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

T. Brixner, F. J. García de Abajo, C. Spindler, and W. Pfeiffer, "Adaptive ultrafast nano-optics in a tight focus," Appl. Phys. B 84, 89-95 (2006).
[CrossRef]

Gerber, G.

T. Brixner and G. Gerber, "Femtosecond polarization pulse shaping," Opt. Lett.  26, 557-559 (2001).
[CrossRef]

T. Baumert, T. Brixner, V. Seyfried, M. Strehle, and G. Gerber, "Femtosecond pulse shaping by an evolutionary algorithm with feedback," Appl. Phys. B 65, 779-782 (1997).
[CrossRef]

Glez, C.

Guild, J. B.

Kiselev, D.

Kurtz, S.

S. Kurtz and T. Perry, "A powder technique for the evaluation of nonlinear optical materials," IEEE J. Quantum Electron. 4, 333-333 (1968).
[CrossRef]

Lambert, Y.

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Le Dantec, R.

J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Glez, and J. -P. Wolf, "Nano-FROG: Frequency resolved optical gating by a nanometric object," Opt. Express 16, 10405-10411 (2008), http://www.opticsinfobase.org/abstract.cfm?URI=oe-16-14-10405.
[CrossRef] [PubMed]

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Le Xuan, L.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

N. Sandeau, L. Le Xuan, C. Zhou, D. Chauvat, J. -F. Roch, and S. Brasselet, "Defocused imaging of second harmonic generation from a single nanocrystal," Opt. Express 15, 16051-16060 (2007), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-15-24-16051.
[CrossRef] [PubMed]

Lin, K. -H.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Lin, K. -J.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Liphard, J.

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Liu, T. -M.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Lozovoy, V. V.

P. Xi, Y. Andegeko, L. R. Weisel, V. V. Lozovoy, and M. Dantus, "Greater Signal and Less Photobleaching in Two-Photon Microscopy with Ultrabroad Bandwidth Femtosecond Pulses," Opt. Commun. 281, 1841-1849 (2008).
[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]

Meshulach, D.

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

Mugnier, Y.

J. Extermann, L. Bonacina, F. Courvoisier, D. Kiselev, Y. Mugnier, R. Le Dantec, C. Glez, and J. -P. Wolf, "Nano-FROG: Frequency resolved optical gating by a nanometric object," Opt. Express 16, 10405-10411 (2008), http://www.opticsinfobase.org/abstract.cfm?URI=oe-16-14-10405.
[CrossRef] [PubMed]

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Nakayama, Y.

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Noordam, L. D.

B. Broers, L. D. Noordam, and H. B. van Lindenvan den Heuvall, "Diffraction and focusing of spectral energy in multiphoton processes," Phys. Rev. A 46, 2749-2756 (1992).
[CrossRef] [PubMed]

Onorato, R. M.

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Oron, D.

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

Pastirk, I.

Pauzauskie, P. J.

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Perruchas, S.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

Perry, T.

S. Kurtz and T. Perry, "A powder technique for the evaluation of nonlinear optical materials," IEEE J. Quantum Electron. 4, 333-333 (1968).
[CrossRef]

Pfeiffer, W.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

T. Brixner, F. J. García de Abajo, C. Spindler, and W. Pfeiffer, "Adaptive ultrafast nano-optics in a tight focus," Appl. Phys. B 84, 89-95 (2006).
[CrossRef]

Rabitz, R.

W. S. Warren, R. Rabitz, and M. Daleh, "Coherent Control of Quantum Dynamics: The Dream Is Alive," Science 259, 1581-1589 (1993).
[CrossRef] [PubMed]

Radenovic, A.

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Radzewicz, C.

P. Wnuk and C. Radzewicz, "Coherent control and dark pulses in second harmonic generation," Opt. Commun. 272, 496-502 (2007).
[CrossRef]

Roch, J. -F.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

N. Sandeau, L. Le Xuan, C. Zhou, D. Chauvat, J. -F. Roch, and S. Brasselet, "Defocused imaging of second harmonic generation from a single nanocrystal," Opt. Express 15, 16051-16060 (2007), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-15-24-16051.
[CrossRef] [PubMed]

Rohmer, M.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

Sandeau, N.

Saykally, R. J.

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Seyfried, V.

T. Baumert, T. Brixner, V. Seyfried, M. Strehle, and G. Gerber, "Femtosecond pulse shaping by an evolutionary algorithm with feedback," Appl. Phys. B 65, 779-782 (1997).
[CrossRef]

Shi, X. -Y.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Shieh, D. -B.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Silberberg, Y.

N. Dudovich, D. Oron, and Y. Silberberg, "Single-pulse coherently controlled nonlinear Raman spectroscopy and microscopy," Nature 418, 512-514 (2002).
[CrossRef] [PubMed]

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

Slablab, A.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

Spindler, C.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

T. Brixner, F. J. García de Abajo, C. Spindler, and W. Pfeiffer, "Adaptive ultrafast nano-optics in a tight focus," Appl. Phys. B 84, 89-95 (2006).
[CrossRef]

Steeb, F.

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[CrossRef] [PubMed]

Strehle, M.

T. Baumert, T. Brixner, V. Seyfried, M. Strehle, and G. Gerber, "Femtosecond pulse shaping by an evolutionary algorithm with feedback," Appl. Phys. B 65, 779-782 (1997).
[CrossRef]

Sun, C. -K.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Tai, S. -P.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Tard, C.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

van den Heuvall, H. B.

B. Broers, L. D. Noordam, and H. B. van Lindenvan den Heuvall, "Diffraction and focusing of spectral energy in multiphoton processes," Phys. Rev. A 46, 2749-2756 (1992).
[CrossRef] [PubMed]

van Linden, H. B.

B. Broers, L. D. Noordam, and H. B. van Lindenvan den Heuvall, "Diffraction and focusing of spectral energy in multiphoton processes," Phys. Rev. A 46, 2749-2756 (1992).
[CrossRef] [PubMed]

Villeval, P.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

Warren, W. S.

W. S. Warren, R. Rabitz, and M. Daleh, "Coherent Control of Quantum Dynamics: The Dream Is Alive," Science 259, 1581-1589 (1993).
[CrossRef] [PubMed]

Webb, W. W.

W. R. Zipfel, R. M. Williams, and W. W. Webb, "Nonlinear magic: multiphoton microscopy in the biosciences," Nature Biotechnol. 21, 1369-1377 (2003).
[CrossRef]

J. B. Guild, C. Xu, and W. W. Webb, "Measurement of group delay dispersion of high numerical aperture objective lenses using two-photon excited fluorescence," Appl. Opt. 36, 397-401 (1997).
[CrossRef] [PubMed]

Weiner, A. M.

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

Weisel, L. R.

P. Xi, Y. Andegeko, L. R. Weisel, V. V. Lozovoy, and M. Dantus, "Greater Signal and Less Photobleaching in Two-Photon Microscopy with Ultrabroad Bandwidth Femtosecond Pulses," Opt. Commun. 281, 1841-1849 (2008).
[CrossRef]

Wen, Y. -C.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Williams, R. M.

W. R. Zipfel, R. M. Williams, and W. W. Webb, "Nonlinear magic: multiphoton microscopy in the biosciences," Nature Biotechnol. 21, 1369-1377 (2003).
[CrossRef]

Wnuk, P.

P. Wnuk and C. Radzewicz, "Coherent control and dark pulses in second harmonic generation," Opt. Commun. 272, 496-502 (2007).
[CrossRef]

Wolf, J. -P.

Wolf, J.-P.

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

Wu, Y.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Xi, P.

P. Xi, Y. Andegeko, L. R. Weisel, V. V. Lozovoy, and M. Dantus, "Greater Signal and Less Photobleaching in Two-Photon Microscopy with Ultrabroad Bandwidth Femtosecond Pulses," Opt. Commun. 281, 1841-1849 (2008).
[CrossRef]

Xu, C.

Yang, P.

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Yu, C. -H.

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Zhou, C.

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

N. Sandeau, L. Le Xuan, C. Zhou, D. Chauvat, J. -F. Roch, and S. Brasselet, "Defocused imaging of second harmonic generation from a single nanocrystal," Opt. Express 15, 16051-16060 (2007), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-15-24-16051.
[CrossRef] [PubMed]

Zipfel, W. R.

W. R. Zipfel, R. M. Williams, and W. W. Webb, "Nonlinear magic: multiphoton microscopy in the biosciences," Nature Biotechnol. 21, 1369-1377 (2003).
[CrossRef]

Adv. Mater. (1)

S. -P. Tai, Y. Wu, D. -B. Shieh, L. -J. Chen, K. -J. Lin, C. -H. Yu, S. -W. Chu, C. -H. Chang, X. -Y. Shi, Y. -C. Wen, K. -H. Lin, T. -M. Liu, and C. -K. Sun, "Molecular Imaging of Cancer Cells Using Plasmon-Resonant-Enhanced Third-Harmonic-Generation in Silver Nanoparticles," Adv. Mater. 19, 4520-4523 (2007).
[CrossRef]

Appl. Opt. (1)

Appl. Phys. B (3)

L. Bonacina, Y. Mugnier, F. Courvoisier, R. Le Dantec, J. Extermann, Y. Lambert, V. Boutou, C. Galez, and J.-P. Wolf, "Polar Fe(IO3)3 nanocrystals as local probes for nonlinear microscopy," Appl. Phys. B 87, 399-403 (2007).
[CrossRef]

T. Baumert, T. Brixner, V. Seyfried, M. Strehle, and G. Gerber, "Femtosecond pulse shaping by an evolutionary algorithm with feedback," Appl. Phys. B 65, 779-782 (1997).
[CrossRef]

T. Brixner, F. J. García de Abajo, C. Spindler, and W. Pfeiffer, "Adaptive ultrafast nano-optics in a tight focus," Appl. Phys. B 84, 89-95 (2006).
[CrossRef]

IEEE J. Quantum Electron. (1)

S. Kurtz and T. Perry, "A powder technique for the evaluation of nonlinear optical materials," IEEE J. Quantum Electron. 4, 333-333 (1968).
[CrossRef]

Nature (4)

M. Aeschlimann, M. Bauer, D. Byer, T. Brixner, F. J. García de Abajo, W. Pfeiffer, M. Rohmer, C. Spindler, and F. Steeb, "Adaptive subwavelength control of nano-optical fields," Nature 446, 301-304 (2007).
[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. Meshulach and Y. Silberberg, "Coherent quantum control of two-photon transitions by a femtosecond laser pulse," Nature 396, 239-242 (1998).
[CrossRef]

Y. Nakayama, P. J. Pauzauskie, A. Radenovic, R. M. Onorato, R. J. Saykally, J. Liphard, and P. Yang, "Tunable nanowire nonlinear optical probe," Nature 447, 1098-1101 (2007).
[CrossRef] [PubMed]

Nature Biotechnol. (1)

W. R. Zipfel, R. M. Williams, and W. W. Webb, "Nonlinear magic: multiphoton microscopy in the biosciences," Nature Biotechnol. 21, 1369-1377 (2003).
[CrossRef]

Opt. Commun. (2)

P. Xi, Y. Andegeko, L. R. Weisel, V. V. Lozovoy, and M. Dantus, "Greater Signal and Less Photobleaching in Two-Photon Microscopy with Ultrabroad Bandwidth Femtosecond Pulses," Opt. Commun. 281, 1841-1849 (2008).
[CrossRef]

P. Wnuk and C. Radzewicz, "Coherent control and dark pulses in second harmonic generation," Opt. Commun. 272, 496-502 (2007).
[CrossRef]

Opt. Express (2)

Opt. Lett. (2)

Phys. Rev. A (1)

B. Broers, L. D. Noordam, and H. B. van Lindenvan den Heuvall, "Diffraction and focusing of spectral energy in multiphoton processes," Phys. Rev. A 46, 2749-2756 (1992).
[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 (1)

W. S. Warren, R. Rabitz, and M. Daleh, "Coherent Control of Quantum Dynamics: The Dream Is Alive," Science 259, 1581-1589 (1993).
[CrossRef] [PubMed]

Small (1)

L. Le Xuan, C. Zhou, A. Slablab, D. Chauvat, C. Tard, S. Perruchas, T. Gacoin, P. Villeval, and J. -F. Roch, "Photostable Second-Harmonic Generation from a Single KTiOPO4 Nanocrystal for Nonlinear Microscopy," Small 4, 1332-1336 (2008).
[CrossRef] [PubMed]

Other (4)

S. Brasselet,V. Le Floc’h, F. Treussart, J. -F. Roch, J. Zyss, E. Botzung-Appert, and A. Ibanez, "In Situ Diagnostics of the Crystalline Nature of Single Organic Nanocrystals by Nonlinear Microscopy," Phys. Rev. Lett. 92, 207401.1-207401.4 (2004).
[CrossRef]

R. W. Boyd, Nonlinear optics, 2nd ed. (Academic Press, 2003).

A Bouhelier, M. Berverhuis, and L. Novotny, "Near-Field Second-Harmonic Generation Induced by Local Field Enhancement," Phys. Rev. Lett. 90, 013903.1-013903.4 (2003).
[CrossRef]

M. Dankwerts and L. Novotny, "Optical Frequency Mixing at Coupled Gold Nanoparticles," Phys. Rev. Lett. 98, 026104.1-026104.4 (2007).

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Figures (5)

Fig. 1.
Fig. 1.

(a) Experimental set-up; OSC- Ti:Sa femtosecond oscillator, DL – prism dispersion line for phase precompression, A – interferometric autocorrelator, PS – pulse shaper with spatial light modulator (SLM), OB – microscope objective, NP – SHG-active nanocrystals deposited on top of a glass plate, TS – translation stage with nanometric resolution, NF – notch filter for second harmonic detection, PCM – photon counting module. (b) Autocorrelation of the shortest precompensated pulse together with the corresponding calculated autocorrelation function. Inset: compensating phase retrieved by the genetic algorithm (GA).

Fig. 2.
Fig. 2.

Detected rate of the SHG from a 100 nm KTP nanocrystal as a function of pulse time duration showing the improvement of the SHG signal with the inverse of the pulse duration.

Fig. 3.
Fig. 3.

SHG maps of the same area of the nanoKTP sample. The maps correspond to excitation with pulse durations τ of (a) 200 fs (SNR=2.5), (b) 100 fs (SNR=4), (c) 65 fs (SNR=4.5) and (d) 13 fs (SNR=16). For each pulse duration both a three-dimensional graph of the SH intensity as well as a normalized two-dimensional map are shown.

Fig. 4.
Fig. 4.

(a) AFM raster scan of the nanoKTP sample (white bar is 1.4 micrometer long) and (b) associated cross section of the selected nanoparticle giving a size of ≈ 120 nm; (c) Associated second harmonic emission with a diffraction-limited spot; (d) Autocorrelation of the 13-fs pulse measured with the same nanoparticle, together with the theoretical autocorrelation of the Fourier limited pulses calculated from the measured laser spectrum.

Fig. 5.
Fig. 5.

Coherent sum frequency generation from a single nano-KTP vs the intensity of the blue band. Inset: corresponding pulse spectrum with two distinctive parts “red” and “blue”. The nonlinear response is detected in the sum-frequency band with an interference filter transmission (spectral transmission shown in red). Note that in the latter case the wavelength scale has been multiplied by two.

Equations (1)

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P i ω R + ω B = ε 0 j , k χ ijk ( 2 ) ( ω R ω B ; ω R , ω B ) E j ω R E k ω B ,

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