Abstract

We propose and demonstrate the use of subharmonically synchronized laser pulses for low-noise lock-in detection in stimulated Raman scattering (SRS) microscopy. In the experiment, Yb-fiber laser pulses at a repetition rate of 38 MHz are successfully synchronized to Ti:sapphire laser pulses at a repetition rate of 76 MHz with a jitter of <8 fs by a two-photon detector and an intra-cavity electro-optic modulator. By using these pulses, high-frequency lock-in detection of SRS signal is accomplished without high-speed optical modulation. The noise level of the lock-in signal is found to be higher than the shot noise limit only by 1.6 dB. We also demonstrate high-contrast, 3D imaging of unlabeled living cells.

© 2010 OSA

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    [CrossRef] [PubMed]

2010 (1)

Y. Ozeki and K. Itoh, “Stimulated Raman scattering microscopy for live-cell imaging with high contrast and high sensitivity,” Laser Phys. 20(5), 1114–1118 (2010).
[CrossRef]

2009 (6)

Y. Ozeki, F. Dake, S. Kajiyama, K. Fukui, and K. Itoh, “Analysis and experimental assessment of the sensitivity of stimulated Raman scattering microscopy,” Opt. Express 17(5), 3651–3658 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-5-3651 .
[CrossRef] [PubMed]

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[CrossRef]

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

T. Minamikawa, M. Hashimoto, K. Fujita, S. Kawata, and T. Araki, “Multi-focus excitation coherent anti-Stokes Raman scattering (CARS) microscopy and its applications for real-time imaging,” Opt. Express 17(12), 9526–9536 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-12-9526 .
[CrossRef] [PubMed]

B. G. Saar, G. R. Holtom, C. W. Freudiger, C. Ackermann, W. Hill, and X. S. Xie, “Intracavity wavelength modulation of an optical parametric oscillator for coherent Raman microscopy,” Opt. Express 17(15), 12532–12539 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-15-12532 .
[CrossRef] [PubMed]

K. Kieu, B. G. Saar, G. R. Holtom, X. S. Xie, and F. W. Wise, “High-power picosecond fiber source for coherent Raman microscopy,” Opt. Lett. 34(13), 2051–2053 (2009), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-34-13-2051 .
[CrossRef] [PubMed]

2008 (2)

C. Heinrich, A. Hofer, A. Ritsch, C. Ciardi, S. Bernet, and M. Ritsch-Marte, “Selective imaging of saturated and unsaturated lipids by wide-field CARS-microscopy,” Opt. Express 16(4), 2699–2708 (2008), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-16-4-2699 .
[CrossRef] [PubMed]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

2007 (1)

D. Fu, T. Ye, T. E. Matthews, G. Yurtsever, and W. S. Warren, “Two-color, two-photon, and excited-state absorption microscopy,” J. Biomed. Opt. 12(5), 054004 (2007).
[CrossRef] [PubMed]

2006 (5)

2005 (3)

2004 (2)

2003 (1)

2002 (2)

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

R. K. Shelton, S. M. Foreman, L.-S. Ma, J. L. Hall, H. C. Kapteyn, M. M. Murnane, M. Notcutt, and J. Ye, “Subfemtosecond timing jitter between two independent, actively synchronized, mode-locked lasers,” Opt. Lett. 27(5), 312–314 (2002), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-27-5-312 .
[CrossRef]

2001 (2)

A. Volkmer, J.-X. Cheng, and X. S. Xie, “Vibrational imaging with high sensitivity via epidetected coherent anti-Stokes Raman scattering microscopy,” Phys. Rev. Lett. 87(2), 023901 (2001).
[CrossRef]

J.-X. Cheng, L. D. Book, and X Sunney Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26(17), 1341–1343 (2001), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-26-17-1341 .
[CrossRef]

2000 (1)

1999 (2)

P. J. Campagnola, M.-D. Wei, A. Lewis, and L. M. Loew, “High-resolution nonlinear optical imaging of live cells by second harmonic generation,” Biophys. J. 77(6), 3341–3349 (1999).
[CrossRef] [PubMed]

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[CrossRef]

1997 (1)

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear scanning laser microscopy by third harmonic generation,” Appl. Phys. Lett. 70(8), 922–924 (1997).
[CrossRef]

1979 (1)

B. F. Levine, C. V. Shank, and J. P. Heritage, “Surface vibrational spectroscopy using stimulated Raman scattering,” IEEE J. Quantum Electron. 15(12), 1418–1432 (1979).
[CrossRef]

Ackermann, C.

Araki, T.

Barad, Y.

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear scanning laser microscopy by third harmonic generation,” Appl. Phys. Lett. 70(8), 922–924 (1997).
[CrossRef]

Bernet, S.

Book, L. D.

Burfeindt, B.

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

Campagnola, P. J.

P. J. Campagnola, M.-D. Wei, A. Lewis, and L. M. Loew, “High-resolution nonlinear optical imaging of live cells by second harmonic generation,” Biophys. J. 77(6), 3341–3349 (1999).
[CrossRef] [PubMed]

Carrasco, S.

Cheng, J.-X.

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

A. Volkmer, J.-X. Cheng, and X. S. Xie, “Vibrational imaging with high sensitivity via epidetected coherent anti-Stokes Raman scattering microscopy,” Phys. Rev. Lett. 87(2), 023901 (2001).
[CrossRef]

J.-X. Cheng, L. D. Book, and X Sunney Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26(17), 1341–1343 (2001), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-26-17-1341 .
[CrossRef]

Chong, S.

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

Ciardi, C.

Côté, D.

C. L. Evans, E. O. Potma, M. Puoris’haag, D. Côté, C. P. Lin, and X. S. Xie, “Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy,” Proc. Natl. Acad. Sci. U.S.A. 102(46), 16807–16812 (2005).
[CrossRef] [PubMed]

Cundiff, S. T.

Dake, F.

Eisenberg, H.

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear scanning laser microscopy by third harmonic generation,” Appl. Phys. Lett. 70(8), 922–924 (1997).
[CrossRef]

Evans, C. L.

Foreman, S. M.

Freudiger, C. W.

B. G. Saar, G. R. Holtom, C. W. Freudiger, C. Ackermann, W. Hill, and X. S. Xie, “Intracavity wavelength modulation of an optical parametric oscillator for coherent Raman microscopy,” Opt. Express 17(15), 12532–12539 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-15-12532 .
[CrossRef] [PubMed]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Fu, D.

D. Fu, T. Ye, T. E. Matthews, G. Yurtsever, and W. S. Warren, “Two-color, two-photon, and excited-state absorption microscopy,” J. Biomed. Opt. 12(5), 054004 (2007).
[CrossRef] [PubMed]

Fujimoto, J. G.

Fujita, K.

T. Minamikawa, M. Hashimoto, K. Fujita, S. Kawata, and T. Araki, “Multi-focus excitation coherent anti-Stokes Raman scattering (CARS) microscopy and its applications for real-time imaging,” Opt. Express 17(12), 9526–9536 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-12-9526 .
[CrossRef] [PubMed]

T. Minamikawa, N. Tanimito, M. Hashimoto, T. Araki, M. Kobayashi, K. Fujita, and S. Kawata, “Jitter reduction of two synchronized picosecond mode-locked lasers using balanced cross-correlator with two-photon detectors,” Appl. Phys. Lett. 89(19), 191101 (2006).
[CrossRef]

Fukui, K.

Ganikhanov, F.

Gopinath, J. T.

Hall, J. L.

Hamaguchi, H. O.

Hashimoto, M.

He, C.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Heinrich, C.

Heritage, J. P.

B. F. Levine, C. V. Shank, and J. P. Heritage, “Surface vibrational spectroscopy using stimulated Raman scattering,” IEEE J. Quantum Electron. 15(12), 1418–1432 (1979).
[CrossRef]

Higashi, T.

Hill, W.

Hofer, A.

Holman, K. W.

Holtom, G. R.

K. Kieu, B. G. Saar, G. R. Holtom, X. S. Xie, and F. W. Wise, “High-power picosecond fiber source for coherent Raman microscopy,” Opt. Lett. 34(13), 2051–2053 (2009), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-34-13-2051 .
[CrossRef] [PubMed]

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

B. G. Saar, G. R. Holtom, C. W. Freudiger, C. Ackermann, W. Hill, and X. S. Xie, “Intracavity wavelength modulation of an optical parametric oscillator for coherent Raman microscopy,” Opt. Express 17(15), 12532–12539 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-15-12532 .
[CrossRef] [PubMed]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[CrossRef]

Horowitz, M.

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear scanning laser microscopy by third harmonic generation,” Appl. Phys. Lett. 70(8), 922–924 (1997).
[CrossRef]

Hudson, D. D.

Ippen, E. P.

Isobe, K.

Itoh, K.

Jones, D. J.

D. D. Hudson, K. W. Holman, R. J. Jones, S. T. Cundiff, J. Ye, and D. J. Jones, “Mode-locked fiber laser frequency-controlled with an intracavity electro-optic modulator,” Opt. Lett. 30(21), 2948–2950 (2005), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-30-21-2948 .
[CrossRef] [PubMed]

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

Jones, R. J.

Kaertner, F. X.

Kajiyama, S.

Kang, J. X.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Kano, H.

Kapteyn, H. C.

Kataoka, S.

Katz, M.

Kawakami, S.

Kawata, S.

Kieu, K.

Kim, J.

Kobayashi, M.

T. Minamikawa, N. Tanimito, M. Hashimoto, T. Araki, M. Kobayashi, K. Fujita, and S. Kawata, “Jitter reduction of two synchronized picosecond mode-locked lasers using balanced cross-correlator with two-photon detectors,” Appl. Phys. Lett. 89(19), 191101 (2006).
[CrossRef]

Kolodziejski, L. A.

Kopf, D.

Kovalev, A.

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[CrossRef]

Kuzucu, O.

Levine, B. F.

B. F. Levine, C. V. Shank, and J. P. Heritage, “Surface vibrational spectroscopy using stimulated Raman scattering,” IEEE J. Quantum Electron. 15(12), 1418–1432 (1979).
[CrossRef]

Lewis, A.

P. J. Campagnola, M.-D. Wei, A. Lewis, and L. M. Loew, “High-resolution nonlinear optical imaging of live cells by second harmonic generation,” Biophys. J. 77(6), 3341–3349 (1999).
[CrossRef] [PubMed]

Lin, C. P.

C. L. Evans, E. O. Potma, M. Puoris’haag, D. Côté, C. P. Lin, and X. S. Xie, “Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy,” Proc. Natl. Acad. Sci. U.S.A. 102(46), 16807–16812 (2005).
[CrossRef] [PubMed]

Loew, L. M.

P. J. Campagnola, M.-D. Wei, A. Lewis, and L. M. Loew, “High-resolution nonlinear optical imaging of live cells by second harmonic generation,” Biophys. J. 77(6), 3341–3349 (1999).
[CrossRef] [PubMed]

Lu, S.

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Ma, L.-S.

Matsunaga, S.

Matthews, T. E.

D. Fu, T. Ye, T. E. Matthews, G. Yurtsever, and W. S. Warren, “Two-color, two-photon, and excited-state absorption microscopy,” J. Biomed. Opt. 12(5), 054004 (2007).
[CrossRef] [PubMed]

Min, W.

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Minamikawa, T.

T. Minamikawa, M. Hashimoto, K. Fujita, S. Kawata, and T. Araki, “Multi-focus excitation coherent anti-Stokes Raman scattering (CARS) microscopy and its applications for real-time imaging,” Opt. Express 17(12), 9526–9536 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-12-9526 .
[CrossRef] [PubMed]

T. Minamikawa, N. Tanimito, M. Hashimoto, T. Araki, M. Kobayashi, K. Fujita, and S. Kawata, “Jitter reduction of two synchronized picosecond mode-locked lasers using balanced cross-correlator with two-photon detectors,” Appl. Phys. Lett. 89(19), 191101 (2006).
[CrossRef]

Murase, R.

Murnane, M. M.

Murphy, T. E.

R. Salem and T. E. Murphy, “Broad-band optical clock recovery system using two-photon absorption,” IEEE Photon. Technol. Lett. 16(9), 2141–2143 (2004).
[CrossRef]

Namiki, S.

S. Takasaka, Y. Ozeki, S. Namiki, and M. Sakano, “External synchronization of 160-GHz optical beat signal by optical phase-locked loop technique,” IEEE Photon. Technol. Lett. 18(23), 2457–2459 (2006).
[CrossRef]

Nandakumar, P.

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[CrossRef]

Notcutt, M.

Ozeki, Y.

Y. Ozeki and K. Itoh, “Stimulated Raman scattering microscopy for live-cell imaging with high contrast and high sensitivity,” Laser Phys. 20(5), 1114–1118 (2010).
[CrossRef]

Y. Ozeki, F. Dake, S. Kajiyama, K. Fukui, and K. Itoh, “Analysis and experimental assessment of the sensitivity of stimulated Raman scattering microscopy,” Opt. Express 17(5), 3651–3658 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-5-3651 .
[CrossRef] [PubMed]

S. Takasaka, Y. Ozeki, S. Namiki, and M. Sakano, “External synchronization of 160-GHz optical beat signal by optical phase-locked loop technique,” IEEE Photon. Technol. Lett. 18(23), 2457–2459 (2006).
[CrossRef]

Pang, Y.

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

Petrich, G. S.

Potma, E. O.

C. L. Evans, E. O. Potma, M. Puoris’haag, D. Côté, C. P. Lin, and X. S. Xie, “Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy,” Proc. Natl. Acad. Sci. U.S.A. 102(46), 16807–16812 (2005).
[CrossRef] [PubMed]

C. L. Evans, E. O. Potma, and X. S. Xie, “Coherent anti-stokes raman scattering spectral interferometry: determination of the real and imaginary components of nonlinear susceptibility χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-29-24-2923 .
[CrossRef]

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

Puoris’haag, M.

C. L. Evans, E. O. Potma, M. Puoris’haag, D. Côté, C. P. Lin, and X. S. Xie, “Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy,” Proc. Natl. Acad. Sci. U.S.A. 102(46), 16807–16812 (2005).
[CrossRef] [PubMed]

Ritsch, A.

Ritsch-Marte, M.

Roy, R.

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

Saar, B. G.

Sakano, M.

S. Takasaka, Y. Ozeki, S. Namiki, and M. Sakano, “External synchronization of 160-GHz optical beat signal by optical phase-locked loop technique,” IEEE Photon. Technol. Lett. 18(23), 2457–2459 (2006).
[CrossRef]

Salem, R.

R. Salem and T. E. Murphy, “Broad-band optical clock recovery system using two-photon absorption,” IEEE Photon. Technol. Lett. 16(9), 2141–2143 (2004).
[CrossRef]

Schibli, T. R.

Seitz, W.

Shank, C. V.

B. F. Levine, C. V. Shank, and J. P. Heritage, “Surface vibrational spectroscopy using stimulated Raman scattering,” IEEE J. Quantum Electron. 15(12), 1418–1432 (1979).
[CrossRef]

Shelton, R. K.

Silberberg, Y.

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear scanning laser microscopy by third harmonic generation,” Appl. Phys. Lett. 70(8), 922–924 (1997).
[CrossRef]

Sunney Xie, X

Sunney Xie, X.

Takasaka, S.

S. Takasaka, Y. Ozeki, S. Namiki, and M. Sakano, “External synchronization of 160-GHz optical beat signal by optical phase-locked loop technique,” IEEE Photon. Technol. Lett. 18(23), 2457–2459 (2006).
[CrossRef]

Tandon, S. N.

Tanimito, N.

T. Minamikawa, N. Tanimito, M. Hashimoto, T. Araki, M. Kobayashi, K. Fujita, and S. Kawata, “Jitter reduction of two synchronized picosecond mode-locked lasers using balanced cross-correlator with two-photon detectors,” Appl. Phys. Lett. 89(19), 191101 (2006).
[CrossRef]

Tsai, J. C.

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Volkmer, A.

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[CrossRef]

A. Volkmer, J.-X. Cheng, and X. S. Xie, “Vibrational imaging with high sensitivity via epidetected coherent anti-Stokes Raman scattering microscopy,” Phys. Rev. Lett. 87(2), 023901 (2001).
[CrossRef]

Warren, W. S.

D. Fu, T. Ye, T. E. Matthews, G. Yurtsever, and W. S. Warren, “Two-color, two-photon, and excited-state absorption microscopy,” J. Biomed. Opt. 12(5), 054004 (2007).
[CrossRef] [PubMed]

Watanabe, W.

Wei, M.-D.

P. J. Campagnola, M.-D. Wei, A. Lewis, and L. M. Loew, “High-resolution nonlinear optical imaging of live cells by second harmonic generation,” Biophys. J. 77(6), 3341–3349 (1999).
[CrossRef] [PubMed]

Wise, F. W.

Xie, X. S.

B. G. Saar, G. R. Holtom, C. W. Freudiger, C. Ackermann, W. Hill, and X. S. Xie, “Intracavity wavelength modulation of an optical parametric oscillator for coherent Raman microscopy,” Opt. Express 17(15), 12532–12539 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-15-12532 .
[CrossRef] [PubMed]

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

K. Kieu, B. G. Saar, G. R. Holtom, X. S. Xie, and F. W. Wise, “High-power picosecond fiber source for coherent Raman microscopy,” Opt. Lett. 34(13), 2051–2053 (2009), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-34-13-2051 .
[CrossRef] [PubMed]

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31(12), 1872–1874 (2006), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-31-12-1872 .
[CrossRef] [PubMed]

C. L. Evans, E. O. Potma, M. Puoris’haag, D. Côté, C. P. Lin, and X. S. Xie, “Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy,” Proc. Natl. Acad. Sci. U.S.A. 102(46), 16807–16812 (2005).
[CrossRef] [PubMed]

C. L. Evans, E. O. Potma, and X. S. Xie, “Coherent anti-stokes raman scattering spectral interferometry: determination of the real and imaginary components of nonlinear susceptibility χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-29-24-2923 .
[CrossRef]

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

A. Volkmer, J.-X. Cheng, and X. S. Xie, “Vibrational imaging with high sensitivity via epidetected coherent anti-Stokes Raman scattering microscopy,” Phys. Rev. Lett. 87(2), 023901 (2001).
[CrossRef]

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[CrossRef]

Ye, J.

Ye, T.

D. Fu, T. Ye, T. E. Matthews, G. Yurtsever, and W. S. Warren, “Two-color, two-photon, and excited-state absorption microscopy,” J. Biomed. Opt. 12(5), 054004 (2007).
[CrossRef] [PubMed]

Yurtsever, G.

D. Fu, T. Ye, T. E. Matthews, G. Yurtsever, and W. S. Warren, “Two-color, two-photon, and excited-state absorption microscopy,” J. Biomed. Opt. 12(5), 054004 (2007).
[CrossRef] [PubMed]

Zumbusch, A.

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[CrossRef]

Appl. Phys. Lett. (2)

Y. Barad, H. Eisenberg, M. Horowitz, and Y. Silberberg, “Nonlinear scanning laser microscopy by third harmonic generation,” Appl. Phys. Lett. 70(8), 922–924 (1997).
[CrossRef]

T. Minamikawa, N. Tanimito, M. Hashimoto, T. Araki, M. Kobayashi, K. Fujita, and S. Kawata, “Jitter reduction of two synchronized picosecond mode-locked lasers using balanced cross-correlator with two-photon detectors,” Appl. Phys. Lett. 89(19), 191101 (2006).
[CrossRef]

Biophys. J. (1)

P. J. Campagnola, M.-D. Wei, A. Lewis, and L. M. Loew, “High-resolution nonlinear optical imaging of live cells by second harmonic generation,” Biophys. J. 77(6), 3341–3349 (1999).
[CrossRef] [PubMed]

IEEE J. Quantum Electron. (1)

B. F. Levine, C. V. Shank, and J. P. Heritage, “Surface vibrational spectroscopy using stimulated Raman scattering,” IEEE J. Quantum Electron. 15(12), 1418–1432 (1979).
[CrossRef]

IEEE Photon. Technol. Lett. (2)

S. Takasaka, Y. Ozeki, S. Namiki, and M. Sakano, “External synchronization of 160-GHz optical beat signal by optical phase-locked loop technique,” IEEE Photon. Technol. Lett. 18(23), 2457–2459 (2006).
[CrossRef]

R. Salem and T. E. Murphy, “Broad-band optical clock recovery system using two-photon absorption,” IEEE Photon. Technol. Lett. 16(9), 2141–2143 (2004).
[CrossRef]

J. Biomed. Opt. (1)

D. Fu, T. Ye, T. E. Matthews, G. Yurtsever, and W. S. Warren, “Two-color, two-photon, and excited-state absorption microscopy,” J. Biomed. Opt. 12(5), 054004 (2007).
[CrossRef] [PubMed]

Laser Phys. (1)

Y. Ozeki and K. Itoh, “Stimulated Raman scattering microscopy for live-cell imaging with high contrast and high sensitivity,” Laser Phys. 20(5), 1114–1118 (2010).
[CrossRef]

N. J. Phys. (1)

P. Nandakumar, A. Kovalev, and A. Volkmer, “Vibrational imaging based on stimulated Raman scattering microscopy,” N. J. Phys. 11(3), 033026 (2009).
[CrossRef]

Nature (1)

W. Min, S. Lu, S. Chong, R. Roy, G. R. Holtom, and X. S. Xie, “Imaging chromophores with undetectable fluorescence by stimulated emission microscopy,” Nature 461(7267), 1105–1109 (2009).
[CrossRef] [PubMed]

Opt. Express (6)

K. Isobe, S. Kataoka, R. Murase, W. Watanabe, T. Higashi, S. Kawakami, S. Matsunaga, K. Fukui, and K. Itoh, “Stimulated parametric emission microscopy,” Opt. Express 14(2), 786–793 (2006), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-14-2-786 .
[CrossRef] [PubMed]

C. Heinrich, A. Hofer, A. Ritsch, C. Ciardi, S. Bernet, and M. Ritsch-Marte, “Selective imaging of saturated and unsaturated lipids by wide-field CARS-microscopy,” Opt. Express 16(4), 2699–2708 (2008), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-16-4-2699 .
[CrossRef] [PubMed]

T. Minamikawa, M. Hashimoto, K. Fujita, S. Kawata, and T. Araki, “Multi-focus excitation coherent anti-Stokes Raman scattering (CARS) microscopy and its applications for real-time imaging,” Opt. Express 17(12), 9526–9536 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-12-9526 .
[CrossRef] [PubMed]

Y. Ozeki, F. Dake, S. Kajiyama, K. Fukui, and K. Itoh, “Analysis and experimental assessment of the sensitivity of stimulated Raman scattering microscopy,” Opt. Express 17(5), 3651–3658 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-5-3651 .
[CrossRef] [PubMed]

H. Kano and H. O. Hamaguchi, “Vibrationally resonant imaging of a single living cell by supercontinuum-based multiplex coherent anti-Stokes Raman scattering microspectroscopy,” Opt. Express 13(4), 1322–1327 (2005), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-13-4-1322 .
[CrossRef] [PubMed]

B. G. Saar, G. R. Holtom, C. W. Freudiger, C. Ackermann, W. Hill, and X. S. Xie, “Intracavity wavelength modulation of an optical parametric oscillator for coherent Raman microscopy,” Opt. Express 17(15), 12532–12539 (2009), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-17-15-12532 .
[CrossRef] [PubMed]

Opt. Lett. (9)

D. D. Hudson, K. W. Holman, R. J. Jones, S. T. Cundiff, J. Ye, and D. J. Jones, “Mode-locked fiber laser frequency-controlled with an intracavity electro-optic modulator,” Opt. Lett. 30(21), 2948–2950 (2005), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-30-21-2948 .
[CrossRef] [PubMed]

R. K. Shelton, S. M. Foreman, L.-S. Ma, J. L. Hall, H. C. Kapteyn, M. M. Murnane, M. Notcutt, and J. Ye, “Subfemtosecond timing jitter between two independent, actively synchronized, mode-locked lasers,” Opt. Lett. 27(5), 312–314 (2002), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-27-5-312 .
[CrossRef]

T. R. Schibli, J. Kim, O. Kuzucu, J. T. Gopinath, S. N. Tandon, G. S. Petrich, L. A. Kolodziejski, J. G. Fujimoto, E. P. Ippen, and F. X. Kaertner, “Attosecond active synchronization of passively mode-locked lasers by balanced cross correlation,” Opt. Lett. 28(11), 947–949 (2003), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-28-11-947 .
[CrossRef] [PubMed]

F. Ganikhanov, S. Carrasco, X. Sunney Xie, M. Katz, W. Seitz, and D. Kopf, “Broadly tunable dual-wavelength light source for coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 31(9), 1292–1294 (2006), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-31-9-1292 .
[CrossRef] [PubMed]

K. Kieu, B. G. Saar, G. R. Holtom, X. S. Xie, and F. W. Wise, “High-power picosecond fiber source for coherent Raman microscopy,” Opt. Lett. 34(13), 2051–2053 (2009), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-34-13-2051 .
[CrossRef] [PubMed]

J.-X. Cheng, L. D. Book, and X Sunney Xie, “Polarization coherent anti-Stokes Raman scattering microscopy,” Opt. Lett. 26(17), 1341–1343 (2001), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-26-17-1341 .
[CrossRef]

C. L. Evans, E. O. Potma, and X. S. Xie, “Coherent anti-stokes raman scattering spectral interferometry: determination of the real and imaginary components of nonlinear susceptibility χ(3) for vibrational microscopy,” Opt. Lett. 29(24), 2923–2925 (2004), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-29-24-2923 .
[CrossRef]

F. Ganikhanov, C. L. Evans, B. G. Saar, and X. S. Xie, “High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy,” Opt. Lett. 31(12), 1872–1874 (2006), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-31-12-1872 .
[CrossRef] [PubMed]

M. Hashimoto, T. Araki, and S. Kawata, “Molecular vibration imaging in the fingerprint region by use of coherent anti-Stokes Raman scattering microscopy with a collinear configuration,” Opt. Lett. 25(24), 1768–1770 (2000), http://www.opticsinfobase.org/ol/abstract.cfm?URI=ol-25-24-1768 .
[CrossRef]

Phys. Rev. Lett. (2)

A. Zumbusch, G. R. Holtom, and X. S. Xie, “Three-dimensional vibrational imaging by coherent anti-Stokes Raman scattering,” Phys. Rev. Lett. 82(20), 4142–4145 (1999).
[CrossRef]

A. Volkmer, J.-X. Cheng, and X. S. Xie, “Vibrational imaging with high sensitivity via epidetected coherent anti-Stokes Raman scattering microscopy,” Phys. Rev. Lett. 87(2), 023901 (2001).
[CrossRef]

Proc. Natl. Acad. Sci. U.S.A. (1)

C. L. Evans, E. O. Potma, M. Puoris’haag, D. Côté, C. P. Lin, and X. S. Xie, “Chemical imaging of tissue in vivo with video-rate coherent anti-Stokes Raman scattering microscopy,” Proc. Natl. Acad. Sci. U.S.A. 102(46), 16807–16812 (2005).
[CrossRef] [PubMed]

Rev. Sci. Instrum. (1)

D. J. Jones, E. O. Potma, J.-X. Cheng, B. Burfeindt, Y. Pang, J. Ye, and X. S. Xie, “Synchronization of two passively mode-locked, picosecond lasers within 20 fs for coherent anti-Stokes Raman scattering microscopy,” Rev. Sci. Instrum. 73(8), 2843–2848 (2002).
[CrossRef]

Science (1)

C. W. Freudiger, W. Min, B. G. Saar, S. Lu, G. R. Holtom, C. He, J. C. Tsai, J. X. Kang, and X. S. Xie, “Label-free biomedical imaging with high sensitivity by stimulated Raman scattering microscopy,” Science 322(5909), 1857–1861 (2008).
[CrossRef] [PubMed]

Other (1)

Y. Kobayashi, X. Zhou, D. Yoshitomi, and K. Torizuka, “Passive timing synchronization between Ti:sapphire laser and Yb-doped fiber laser,” in Conference on Lasers and Electro-Optics/Quantum Electronics and Laser Science Conference and Photonic Applications Systems Technologies, OSA Technical Digest (CD) (Optical Society of America, 2008), paper CML6. http://www.opticsinfobase.org/abstract.cfm?URI=CLEO-2008-CML6 .

Supplementary Material (2)

» Media 1: MPG (11850 KB)     
» Media 2: MPG (11329 KB)     

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Figures (5)

Fig. 1
Fig. 1

Principle of lock-in detection of SRS signal employing (a) an intensity modulator (IM) and (b) subharmonically synchronized pulse sources demonstrated in this paper.

Fig. 2
Fig. 2

Experimental setup. M: mirror, DM: dichroic mirror, SM: switchable mirror, PBS: polarization beam splitter, YDF: Yb-doped fiber, G: diffraction grating, LD: 980-nm pump laser diode, PM: in-line phase modulator, PD: photodiode, L: lens, OB: objective lens, F: short-pass filter.

Fig. 3
Fig. 3

Results of the synchronization experiment. (a) Intensity cross-correlation measured by the GaAsP PD. (b) The waveform of the error signal measured when the loop was closed. (c) Solid line: in-loop error signal (upper) and out-of-loop error signal (lower). Red broken line: probability densities. (d) Solid line: spectral densities of the in-loop (gray) and out-of-loop (red) error signals. Broken line: integrated jitter. (e) Long-term out-of-loop jitter measured for 30 min.

Fig. 4
Fig. 4

(a) SRS spectrum of a polystyrene bead with a diameter of 10 µm. (b) Circle: noise level of the lock-in signal as a function of photocurrent of Si-PD. Cross: corresponding noise level in our previous setup. Green line: theoretical shot noise level given by Eq. (1). Broken line: circuit noise.

Fig. 5
Fig. 5

3D SRS images of (a) a cultured tobacco BY-2 cell (Media 1), and (b) a cultured HeLa cell (Media 2). The pixel dwell time: (a) 0.2 ms, (b) 0.5 ms. Number of pixels: (a) 300 x 300 x 40, (b) 400 x 400 x 32. The size of the observed region: (a) 60 x 60 x 40 µm3, (b) 40 x 40 x 10 µm3.

Equations (15)

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v shot = RG 2 qi τ ,
Δ f < B Δ t / T ,
v ( t ) = R η q h ν m { h ( t m T ) Δ t [ I 0 δ I 2 ( 1 + cos ω 0 m T ) ] } ,
h ( t ) d t = 1 .
v L = 2 τ 0 τ v ( t ' ) cos ω 0 t ' d t ' ,
v L = 2 τ R η q h ν 0 τ cos ω 0 t ' m { h ( t ' m T ) Δ t [ I 0 δ I 2 ( 1 + cos ω 0 m T ) ] } d t ' = 2 τ R η q h ν cos ω 0 t ' m = 0 N 1 { h ( t ' m T ) Δ t [ I 0 δ I 2 ( 1 + cos ω 0 m T ) ] } = 2 R η q Δ t h ν τ [ I 0 δ I 2 ] m = 0 N 1 h ( t ' ) cos ω 0 ( t ' + m T ) d t ' 2 R η q Δ t δ I 2 h ν τ m = 0 N 1 h ( t ' ) cos ω 0 ( t ' + m T ) cos m ω 0 T d t ' ,
2 R η q Δ t h ν τ [ I 0 δ I 2 ] m = 0 N 1 h ( t ' ) cos ω 0 ( t ' + m T ) d t ' = 2 R η q Δ t h ν τ [ I 0 δ I 2 ] m = 0 N 1 [ cos m ω 0 T Re H ( ω 0 ) + sin m ω 0 T Im H ( ω 0 ) ] = 0 ,
H ( ω ) = h ( t ) e i ω t d t
v L = 2 R η q Δ t δ I 2 h ν τ m = 0 N 1 h ( t ' ) cos ω 0 ( t ' + m T ) cos m ω 0 T d t ' = 2 R η q Δ t δ I 4 τ h ν m = 0 N 1 [ Re H ( ω ) cos 2 m T + Im H ( ω ) sin 2 m T + Re H ( ω ) ] = { 2 R η q Δ t δ I 2 h ν T Re H ( ω ) , ω 0 = ω rep 2 , 2 R η q Δ t δ I 4 h ν T Re H ( ω ) , 0 < ω 0 < ω rep 2 ,
Δ v L = 2 R η q Δ t h ν τ m = 0 N 1 Δ I m h ( t ' ) cos ω 0 ( t ' + m T ) d t ' = 2 R η q Δ t h ν τ m = 0 N 1 Δ I m [ Re H ( ω ) cos m ω 0 T + Im H ( ω ) sin m ω 0 T ] .
Δ v L 2 ¯ = [ 2 R η q Δ t h ν τ ] 2 m = 0 N 1 Δ I m 2 { [ Re H ( ω ) ] 2 cos 2 m ω 0 T + [ Im H ( ω ) ] 2 sin 2 m ω 0 T } = [ 2 R η q Δ t h ν τ ] 2 m = 0 N 1 Δ I m 2 { [ Re H ( ω ) ] 2 1 + cos 2 m ω 0 T 2 + [ Im H ( ω ) ] 2 1 cos 2 m ω 0 T 2 } = { [ 2 R η q Δ t h ν τ ] 2 [ Re H ( ω ) ] 2 m = 0 N 1 Δ I m 2 , ω 0 = ω rep 2 , [ 2 R η q Δ t h ν τ ] 2 | H ( ω ) | 2 2 m = 0 N 1 Δ I m 2 , 0 < ω 0 < ω rep 2 .
Δ I m 2 ¯ = h ν I 0 η Δ t .
Δ v L 2 ¯ = { R q 2 η Δ t I 0 h ν τ T | Re H ( ω ) | , ω 0 = ω rep 2 , R q η Δ t I 0 h ν τ T | H ( ω ) | , 0 < ω 0 < ω rep 2 .
v L 2 Δ v L 2 ¯ = { δ I 2 η Δ t τ 4 h ν T I 0 , ω 0 = ω rep 2 , δ I 2 η Δ t τ 8 h ν T I 0 | Re H ( ω ) H ( ω ) | 2 , 0 < ω 0 < ω rep 2 .
Δ v L 2 ¯ = { R 2 q i 0 τ Re H ( ω ) ω 0 = ω rep 2 , R q i 0 τ | H ( ω ) | 0 < ω 0 < ω rep 2 ,

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