Abstract

We employ the finite-difference time-domain (FDTD) technique as a numerical approach to studying the effects of polarization, scatterers’ sizes and orientations on near-field coherent anti-Stokes Raman scattering (CARS) microscopy imaging. The results show that to acquire better image contrast and larger near-field CARS signals, the scatterers with diameters of less than three-eighths of the pump field wavelength (λp) are preferable to be oriented along the polarization direction of the excitation light fields. It is also found that when the scatterers’ sizes are smaller than half a wavelength of the pump field, the perpendicular polarization component of the induced near-field CARS radiations is strictly confined within the regions at the scatterer-water interface or the subsurface of scatterers, yielding a high image contrast (up to 200) with a spatial resolution of λp/16. This study indicates that perpendicular polarization components of near-field CARS microscopy could be used to uncover very fine structures of intra- and/or inter- cellular organelles in cells with nanoscale resolutions.

© 2009 Optical Society of America

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  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. 102, 16807-16812 (2005).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  4. E. Potma, W. P. de Boeij, P. J. van Haastert, and D. A. Wiersma, "Real-time visualization of intracellular hydrodynamics in single living cells," Proc. Natl. Acad. Sci. 98, 1577-1582 (2001).
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  7. X. Nan, E. O. Potma, and X. S. Xie, "Nonperturbative chemical imaging of organelle transport in living cells with coherent anti-Stokes Raman scattering microscopy," Biophys. J. 91, 728-735 (2006).
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    [CrossRef] [PubMed]
  10. G. W. Wurpel, H. A. Rinia, and M. Muller, "Imaging orientational order and lipid density in multilamellar vescles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (2005).
    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef]
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    [CrossRef]
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    [CrossRef] [PubMed]
  25. V. V. Krishnamachari and E. O. Potma, "Focus-engineered coherent anti-Stokes Raman scattering microscopy: a numerical investigation," J. Opt. Soc. Am. A 24, 1138-1147 (2007).
    [CrossRef]
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2008 (4)

2007 (4)

2006 (4)

Y. Saito, M. Motohashi, N. Hayazawa, M. Iyoki, and S. Kawata, "Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode," Appl. Phys. Lett. 88, 143109 (2006).
[CrossRef]

N. Djaker, D. Gachet, N. Sandeau, P. F. Lenne, and R. Hervé, "Refractive effects in coherent anti-Stokes Raman scattering microscopy," Appl. Opt. 45, 7005-7011 (2006).
[CrossRef] [PubMed]

X. Nan, E. O. Potma, and X. S. Xie, "Nonperturbative chemical imaging of organelle transport in living cells with coherent anti-Stokes Raman scattering microscopy," Biophys. J. 91, 728-735 (2006).
[CrossRef] [PubMed]

X. S. Xie, J. Yu, and W. Yang, "Living cells as test tubes," Science 312, 228-230 (2006).
[CrossRef] [PubMed]

2005 (6)

G. W. Wurpel, H. A. Rinia, and M. Muller, "Imaging orientational order and lipid density in multilamellar vescles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (2005).
[CrossRef] [PubMed]

H. Wang. Y. Fu, P. Zickmund, R. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J 89, 581-591 (2005).
[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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

B. Jia, X. Gan, and M. Gu, "Direct measurement of a radially polarized focused evanescent field facilitated by a single LCD," Opt. Express 13, 6821-6827 (2005).
[CrossRef] [PubMed]

B. Jia, X. Gan, and M. Gu, "Direct observation of a pure focused evanescent field of a high numerical aperture objective lens by scanning near-field optical microscopy," Appl. Phys. Lett. 86, 131110 (2005).
[CrossRef]

A. Volkmer, "Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy," J. Phys. D: Appl. Phys. 38, 59-81 (2005).
[CrossRef]

2004 (3)

S. Kawata, I. Yasushi, and I. Taro, "Near-field optics and spectroscopy for molecular nano-imaging," Sci. Progress 87, 25-49 (2004).
[CrossRef]

T. Ichimura, N. Hayazawa, M. Hashimoto, Y. Inouye, and S. Kawata, "Tip-enhanced coherent anti-Stokes Raman scattering for vibrational nano-imaging," Phys. Rev. Lett. 92, 220801 (2004).
[CrossRef] [PubMed]

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microcopy: instrumentation, theory, and applications," J. Phys. Chem. B 108, 827-840 (2004).
[CrossRef]

2003 (1)

J. X. Cheng, S. Pautot, D. A. Weitz, and X. S. Xie, "Ordering of water molecules between phospholipid bilayers visualized by coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. 100, 9826-9830 (2003).
[CrossRef] [PubMed]

2002 (2)

J. X. Cheng and X. S. Xie, "Green’s function formulation for third-harmonic generation microscopy," J. Opt. Soc. Am. B 19, 1604-1610 (2002).
[CrossRef]

R. D. Schaller, J. Ziegelbauer, L. F. Lee, L. H. Haber, and R. J. Saykally, "Chemically selective imaging of subcellular structure in human hepatocytes with coherent anti-stokes Raman scattering (CARS) near-field scanning optical microscopy (NSOM)," J. Phys. Chem. B 106, 8489-8492 (2002).
[CrossRef]

2001 (1)

E. Potma, W. P. de Boeij, P. J. van Haastert, and D. A. Wiersma, "Real-time visualization of intracellular hydrodynamics in single living cells," Proc. Natl. Acad. Sci. 98, 1577-1582 (2001).
[CrossRef] [PubMed]

1999 (1)

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

1994 (1)

D. Courjon and C. Bainier, "Near field microscopy and near field optics," Rep. Prog. Phys. 57, 989-1028 (1994).
[CrossRef]

1992 (1)

K. Takeda, Y. Ito, and C. Munakata, "Simultaneous measurement of size and refractive index of a fine particle in flowing liquid," Meas. Sci. Technol. 3, 27-32 (1992).
[CrossRef]

1966 (1)

K. S. Yee, "Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media," IEEE Trans. Antennas Propag. 14, 302-307 (1966).
[CrossRef]

Bainier, C.

D. Courjon and C. Bainier, "Near field microscopy and near field optics," Rep. Prog. Phys. 57, 989-1028 (1994).
[CrossRef]

Cheng, J. X.

T. T. Le, I. M. Langohr, M. J. Locker, M. Sturek, and J. X. Cheng, "Label-free molecular imaging of atherosclerotic lesions using multimodal nonlinear optical microscopy," J. Biomed. Opt. 12, 054007 (2007).
[CrossRef] [PubMed]

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microcopy: instrumentation, theory, and applications," J. Phys. Chem. B 108, 827-840 (2004).
[CrossRef]

J. X. Cheng, S. Pautot, D. A. Weitz, and X. S. Xie, "Ordering of water molecules between phospholipid bilayers visualized by coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. 100, 9826-9830 (2003).
[CrossRef] [PubMed]

J. X. Cheng and X. S. Xie, "Green’s function formulation for third-harmonic generation microscopy," J. Opt. Soc. Am. B 19, 1604-1610 (2002).
[CrossRef]

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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Courjon, D.

D. Courjon and C. Bainier, "Near field microscopy and near field optics," Rep. Prog. Phys. 57, 989-1028 (1994).
[CrossRef]

de Boeij, W. P.

E. Potma, W. P. de Boeij, P. J. van Haastert, and D. A. Wiersma, "Real-time visualization of intracellular hydrodynamics in single living cells," Proc. Natl. Acad. Sci. 98, 1577-1582 (2001).
[CrossRef] [PubMed]

Djaker, N.

Evans, C. L.

C. L. Evans, X. Xu, S. Kesari, X. S. Xie, S. T. C. Wong, and G. S. Young, "Chemically-selective imaging of brain structures with CARS microscopy," Opt. Express 15, 12076-12087 (2007).
[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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Gachet, D.

Gan, X.

B. Jia, X. Gan, and M. Gu, "Direct observation of a pure focused evanescent field of a high numerical aperture objective lens by scanning near-field optical microscopy," Appl. Phys. Lett. 86, 131110 (2005).
[CrossRef]

B. Jia, X. Gan, and M. Gu, "Direct measurement of a radially polarized focused evanescent field facilitated by a single LCD," Opt. Express 13, 6821-6827 (2005).
[CrossRef] [PubMed]

Gu, M.

B. Jia, X. Gan, and M. Gu, "Direct measurement of a radially polarized focused evanescent field facilitated by a single LCD," Opt. Express 13, 6821-6827 (2005).
[CrossRef] [PubMed]

B. Jia, X. Gan, and M. Gu, "Direct observation of a pure focused evanescent field of a high numerical aperture objective lens by scanning near-field optical microscopy," Appl. Phys. Lett. 86, 131110 (2005).
[CrossRef]

Haber, L. H.

R. D. Schaller, J. Ziegelbauer, L. F. Lee, L. H. Haber, and R. J. Saykally, "Chemically selective imaging of subcellular structure in human hepatocytes with coherent anti-stokes Raman scattering (CARS) near-field scanning optical microscopy (NSOM)," J. Phys. Chem. B 106, 8489-8492 (2002).
[CrossRef]

Hashimoto, M.

T. Ichimura, N. Hayazawa, M. Hashimoto, Y. Inouye, and S. Kawata, "Tip-enhanced coherent anti-Stokes Raman scattering for vibrational nano-imaging," Phys. Rev. Lett. 92, 220801 (2004).
[CrossRef] [PubMed]

Hayazawa, N.

Y. Saito, M. Motohashi, N. Hayazawa, M. Iyoki, and S. Kawata, "Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode," Appl. Phys. Lett. 88, 143109 (2006).
[CrossRef]

T. Ichimura, N. Hayazawa, M. Hashimoto, Y. Inouye, and S. Kawata, "Tip-enhanced coherent anti-Stokes Raman scattering for vibrational nano-imaging," Phys. Rev. Lett. 92, 220801 (2004).
[CrossRef] [PubMed]

Hervé, R.

Holtom, G. R.

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

Huang, Z.

Hutmacher, D. W.

Ichimura, T.

T. Ichimura, N. Hayazawa, M. Hashimoto, Y. Inouye, and S. Kawata, "Tip-enhanced coherent anti-Stokes Raman scattering for vibrational nano-imaging," Phys. Rev. Lett. 92, 220801 (2004).
[CrossRef] [PubMed]

Inouye, Y.

T. Ichimura, N. Hayazawa, M. Hashimoto, Y. Inouye, and S. Kawata, "Tip-enhanced coherent anti-Stokes Raman scattering for vibrational nano-imaging," Phys. Rev. Lett. 92, 220801 (2004).
[CrossRef] [PubMed]

Ito, Y.

K. Takeda, Y. Ito, and C. Munakata, "Simultaneous measurement of size and refractive index of a fine particle in flowing liquid," Meas. Sci. Technol. 3, 27-32 (1992).
[CrossRef]

Iyoki, M.

Y. Saito, M. Motohashi, N. Hayazawa, M. Iyoki, and S. Kawata, "Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode," Appl. Phys. Lett. 88, 143109 (2006).
[CrossRef]

Jia, B.

B. Jia, X. Gan, and M. Gu, "Direct observation of a pure focused evanescent field of a high numerical aperture objective lens by scanning near-field optical microscopy," Appl. Phys. Lett. 86, 131110 (2005).
[CrossRef]

B. Jia, X. Gan, and M. Gu, "Direct measurement of a radially polarized focused evanescent field facilitated by a single LCD," Opt. Express 13, 6821-6827 (2005).
[CrossRef] [PubMed]

Kawata, S.

Y. Saito, M. Motohashi, N. Hayazawa, M. Iyoki, and S. Kawata, "Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode," Appl. Phys. Lett. 88, 143109 (2006).
[CrossRef]

S. Kawata, I. Yasushi, and I. Taro, "Near-field optics and spectroscopy for molecular nano-imaging," Sci. Progress 87, 25-49 (2004).
[CrossRef]

T. Ichimura, N. Hayazawa, M. Hashimoto, Y. Inouye, and S. Kawata, "Tip-enhanced coherent anti-Stokes Raman scattering for vibrational nano-imaging," Phys. Rev. Lett. 92, 220801 (2004).
[CrossRef] [PubMed]

Kesari, S.

Krishnamachari, V. V.

Langohr, I. M.

T. T. Le, I. M. Langohr, M. J. Locker, M. Sturek, and J. X. Cheng, "Label-free molecular imaging of atherosclerotic lesions using multimodal nonlinear optical microscopy," J. Biomed. Opt. 12, 054007 (2007).
[CrossRef] [PubMed]

Le, T. T.

T. T. Le, I. M. Langohr, M. J. Locker, M. Sturek, and J. X. Cheng, "Label-free molecular imaging of atherosclerotic lesions using multimodal nonlinear optical microscopy," J. Biomed. Opt. 12, 054007 (2007).
[CrossRef] [PubMed]

Lee, L. F.

R. D. Schaller, J. Ziegelbauer, L. F. Lee, L. H. Haber, and R. J. Saykally, "Chemically selective imaging of subcellular structure in human hepatocytes with coherent anti-stokes Raman scattering (CARS) near-field scanning optical microscopy (NSOM)," J. Phys. Chem. B 106, 8489-8492 (2002).
[CrossRef]

Lenne, P. F.

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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Liu, C.

Locker, M. J.

T. T. Le, I. M. Langohr, M. J. Locker, M. Sturek, and J. X. Cheng, "Label-free molecular imaging of atherosclerotic lesions using multimodal nonlinear optical microscopy," J. Biomed. Opt. 12, 054007 (2007).
[CrossRef] [PubMed]

Lu, F.

Motohashi, M.

Y. Saito, M. Motohashi, N. Hayazawa, M. Iyoki, and S. Kawata, "Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode," Appl. Phys. Lett. 88, 143109 (2006).
[CrossRef]

Muller, M.

G. W. Wurpel, H. A. Rinia, and M. Muller, "Imaging orientational order and lipid density in multilamellar vescles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (2005).
[CrossRef] [PubMed]

Munakata, C.

K. Takeda, Y. Ito, and C. Munakata, "Simultaneous measurement of size and refractive index of a fine particle in flowing liquid," Meas. Sci. Technol. 3, 27-32 (1992).
[CrossRef]

Nan, X.

X. Nan, E. O. Potma, and X. S. Xie, "Nonperturbative chemical imaging of organelle transport in living cells with coherent anti-Stokes Raman scattering microscopy," Biophys. J. 91, 728-735 (2006).
[CrossRef] [PubMed]

Pautot, S.

J. X. Cheng, S. Pautot, D. A. Weitz, and X. S. Xie, "Ordering of water molecules between phospholipid bilayers visualized by coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. 100, 9826-9830 (2003).
[CrossRef] [PubMed]

Potma, E.

E. Potma, W. P. de Boeij, P. J. van Haastert, and D. A. Wiersma, "Real-time visualization of intracellular hydrodynamics in single living cells," Proc. Natl. Acad. Sci. 98, 1577-1582 (2001).
[CrossRef] [PubMed]

Potma, E. O.

V. V. Krishnamachari and E. O. Potma, "Focus-engineered coherent anti-Stokes Raman scattering microscopy: a numerical investigation," J. Opt. Soc. Am. A 24, 1138-1147 (2007).
[CrossRef]

X. Nan, E. O. Potma, and X. S. Xie, "Nonperturbative chemical imaging of organelle transport in living cells with coherent anti-Stokes Raman scattering microscopy," Biophys. J. 91, 728-735 (2006).
[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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

Rinia, H. A.

G. W. Wurpel, H. A. Rinia, and M. Muller, "Imaging orientational order and lipid density in multilamellar vescles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (2005).
[CrossRef] [PubMed]

Saito, Y.

Y. Saito, M. Motohashi, N. Hayazawa, M. Iyoki, and S. Kawata, "Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode," Appl. Phys. Lett. 88, 143109 (2006).
[CrossRef]

Sandeau, N.

Saykally, R. J.

R. D. Schaller, J. Ziegelbauer, L. F. Lee, L. H. Haber, and R. J. Saykally, "Chemically selective imaging of subcellular structure in human hepatocytes with coherent anti-stokes Raman scattering (CARS) near-field scanning optical microscopy (NSOM)," J. Phys. Chem. B 106, 8489-8492 (2002).
[CrossRef]

Schaller, R. D.

R. D. Schaller, J. Ziegelbauer, L. F. Lee, L. H. Haber, and R. J. Saykally, "Chemically selective imaging of subcellular structure in human hepatocytes with coherent anti-stokes Raman scattering (CARS) near-field scanning optical microscopy (NSOM)," J. Phys. Chem. B 106, 8489-8492 (2002).
[CrossRef]

Sheppard, C.

Sturek, M.

T. T. Le, I. M. Langohr, M. J. Locker, M. Sturek, and J. X. Cheng, "Label-free molecular imaging of atherosclerotic lesions using multimodal nonlinear optical microscopy," J. Biomed. Opt. 12, 054007 (2007).
[CrossRef] [PubMed]

Takeda, K.

K. Takeda, Y. Ito, and C. Munakata, "Simultaneous measurement of size and refractive index of a fine particle in flowing liquid," Meas. Sci. Technol. 3, 27-32 (1992).
[CrossRef]

Taro, I.

S. Kawata, I. Yasushi, and I. Taro, "Near-field optics and spectroscopy for molecular nano-imaging," Sci. Progress 87, 25-49 (2004).
[CrossRef]

van Haastert, P. J.

E. Potma, W. P. de Boeij, P. J. van Haastert, and D. A. Wiersma, "Real-time visualization of intracellular hydrodynamics in single living cells," Proc. Natl. Acad. Sci. 98, 1577-1582 (2001).
[CrossRef] [PubMed]

Volkmer, A.

A. Volkmer, "Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy," J. Phys. D: Appl. Phys. 38, 59-81 (2005).
[CrossRef]

Wang, H.

H. Wang. Y. Fu, P. Zickmund, R. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J 89, 581-591 (2005).
[CrossRef] [PubMed]

Weitz, D. A.

J. X. Cheng, S. Pautot, D. A. Weitz, and X. S. Xie, "Ordering of water molecules between phospholipid bilayers visualized by coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. 100, 9826-9830 (2003).
[CrossRef] [PubMed]

Wiersma, D. A.

E. Potma, W. P. de Boeij, P. J. van Haastert, and D. A. Wiersma, "Real-time visualization of intracellular hydrodynamics in single living cells," Proc. Natl. Acad. Sci. 98, 1577-1582 (2001).
[CrossRef] [PubMed]

Wong, S. T. C.

Wurpel, G. W.

G. W. Wurpel, H. A. Rinia, and M. Muller, "Imaging orientational order and lipid density in multilamellar vescles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (2005).
[CrossRef] [PubMed]

Xie, X. S.

C. L. Evans, X. Xu, S. Kesari, X. S. Xie, S. T. C. Wong, and G. S. Young, "Chemically-selective imaging of brain structures with CARS microscopy," Opt. Express 15, 12076-12087 (2007).
[CrossRef] [PubMed]

X. S. Xie, J. Yu, and W. Yang, "Living cells as test tubes," Science 312, 228-230 (2006).
[CrossRef] [PubMed]

X. Nan, E. O. Potma, and X. S. Xie, "Nonperturbative chemical imaging of organelle transport in living cells with coherent anti-Stokes Raman scattering microscopy," Biophys. J. 91, 728-735 (2006).
[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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microcopy: instrumentation, theory, and applications," J. Phys. Chem. B 108, 827-840 (2004).
[CrossRef]

J. X. Cheng, S. Pautot, D. A. Weitz, and X. S. Xie, "Ordering of water molecules between phospholipid bilayers visualized by coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. 100, 9826-9830 (2003).
[CrossRef] [PubMed]

J. X. Cheng and X. S. Xie, "Green’s function formulation for third-harmonic generation microscopy," J. Opt. Soc. Am. B 19, 1604-1610 (2002).
[CrossRef]

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

Xu, X.

Yang, W.

X. S. Xie, J. Yu, and W. Yang, "Living cells as test tubes," Science 312, 228-230 (2006).
[CrossRef] [PubMed]

Yasushi, I.

S. Kawata, I. Yasushi, and I. Taro, "Near-field optics and spectroscopy for molecular nano-imaging," Sci. Progress 87, 25-49 (2004).
[CrossRef]

Yee, K. S.

K. S. Yee, "Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media," IEEE Trans. Antennas Propag. 14, 302-307 (1966).
[CrossRef]

Young, G. S.

Yu, J.

X. S. Xie, J. Yu, and W. Yang, "Living cells as test tubes," Science 312, 228-230 (2006).
[CrossRef] [PubMed]

Zheng, W.

Ziegelbauer, J.

R. D. Schaller, J. Ziegelbauer, L. F. Lee, L. H. Haber, and R. J. Saykally, "Chemically selective imaging of subcellular structure in human hepatocytes with coherent anti-stokes Raman scattering (CARS) near-field scanning optical microscopy (NSOM)," J. Phys. Chem. B 106, 8489-8492 (2002).
[CrossRef]

Zumbushch, A.

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

Appl. Opt. (1)

Appl. Phys. Lett. (3)

Y. Saito, M. Motohashi, N. Hayazawa, M. Iyoki, and S. Kawata, "Nanoscale characterization of strained silicon by tip-enhanced Raman spectroscope in reflection mode," Appl. Phys. Lett. 88, 143109 (2006).
[CrossRef]

B. Jia, X. Gan, and M. Gu, "Direct observation of a pure focused evanescent field of a high numerical aperture objective lens by scanning near-field optical microscopy," Appl. Phys. Lett. 86, 131110 (2005).
[CrossRef]

F. Lu, W. Zheng, and Z. Huang, "Heterodyne polarization coherent anti-Stokes Raman scattering microscopy," Appl. Phys. Lett. 92, 123901 (2008).
[CrossRef]

Biophys. J (1)

H. Wang. Y. Fu, P. Zickmund, R. Shi, and J. X. Cheng, "Coherent anti-Stokes Raman scattering imaging of axonal myelin in live spinal tissues," Biophys. J 89, 581-591 (2005).
[CrossRef] [PubMed]

Biophys. J. (1)

X. Nan, E. O. Potma, and X. S. Xie, "Nonperturbative chemical imaging of organelle transport in living cells with coherent anti-Stokes Raman scattering microscopy," Biophys. J. 91, 728-735 (2006).
[CrossRef] [PubMed]

IEEE Trans. Antennas Propag. (1)

K. S. Yee, "Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media," IEEE Trans. Antennas Propag. 14, 302-307 (1966).
[CrossRef]

J. Biomed. Opt. (1)

T. T. Le, I. M. Langohr, M. J. Locker, M. Sturek, and J. X. Cheng, "Label-free molecular imaging of atherosclerotic lesions using multimodal nonlinear optical microscopy," J. Biomed. Opt. 12, 054007 (2007).
[CrossRef] [PubMed]

J. Microsc. (1)

G. W. Wurpel, H. A. Rinia, and M. Muller, "Imaging orientational order and lipid density in multilamellar vescles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (2005).
[CrossRef] [PubMed]

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

J. Opt. Soc. Am. B (2)

J. Phys. Chem. B (2)

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microcopy: instrumentation, theory, and applications," J. Phys. Chem. B 108, 827-840 (2004).
[CrossRef]

R. D. Schaller, J. Ziegelbauer, L. F. Lee, L. H. Haber, and R. J. Saykally, "Chemically selective imaging of subcellular structure in human hepatocytes with coherent anti-stokes Raman scattering (CARS) near-field scanning optical microscopy (NSOM)," J. Phys. Chem. B 106, 8489-8492 (2002).
[CrossRef]

J. Phys. D: Appl. Phys. (1)

A. Volkmer, "Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy," J. Phys. D: Appl. Phys. 38, 59-81 (2005).
[CrossRef]

Meas. Sci. Technol. (1)

K. Takeda, Y. Ito, and C. Munakata, "Simultaneous measurement of size and refractive index of a fine particle in flowing liquid," Meas. Sci. Technol. 3, 27-32 (1992).
[CrossRef]

Opt. Express (3)

Opt. Lett. (2)

Phys. Rev. Lett. (2)

T. Ichimura, N. Hayazawa, M. Hashimoto, Y. Inouye, and S. Kawata, "Tip-enhanced coherent anti-Stokes Raman scattering for vibrational nano-imaging," Phys. Rev. Lett. 92, 220801 (2004).
[CrossRef] [PubMed]

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

Proc. Natl. Acad. Sci. (3)

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. 102, 16807-16812 (2005).
[CrossRef] [PubMed]

E. Potma, W. P. de Boeij, P. J. van Haastert, and D. A. Wiersma, "Real-time visualization of intracellular hydrodynamics in single living cells," Proc. Natl. Acad. Sci. 98, 1577-1582 (2001).
[CrossRef] [PubMed]

J. X. Cheng, S. Pautot, D. A. Weitz, and X. S. Xie, "Ordering of water molecules between phospholipid bilayers visualized by coherent anti-Stokes Raman scattering microscopy," Proc. Natl. Acad. Sci. 100, 9826-9830 (2003).
[CrossRef] [PubMed]

Rep. Prog. Phys. (1)

D. Courjon and C. Bainier, "Near field microscopy and near field optics," Rep. Prog. Phys. 57, 989-1028 (1994).
[CrossRef]

Sci. Progress (1)

S. Kawata, I. Yasushi, and I. Taro, "Near-field optics and spectroscopy for molecular nano-imaging," Sci. Progress 87, 25-49 (2004).
[CrossRef]

Science (1)

X. S. Xie, J. Yu, and W. Yang, "Living cells as test tubes," Science 312, 228-230 (2006).
[CrossRef] [PubMed]

Other (3)

M. Born and E. Wolf, Principles of Optics (7th edition, Cambridge University Press, Cambridge, 1999).

A. Taflove, Computational Electrodynamics: The Finite-Difference Time-Domain Method (Artech House, Boston, 1995).

R. L. Sutherland, Handbook of Nonlinear Optics (Marcel Dekker, New York, 2003).
[CrossRef]

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Figures (6)

Fig. 1.
Fig. 1.

Schematic diagram of CARS experiments (a) and three different configurations of nanoparticles’ orientations with respect to the polarizations of the pump and Stokes light fields (b, c, d).

Fig. 2.
Fig. 2.

Distributions of the focused pump field Ey with y-polarization in the y-z plane for the two scatterers arranged in the z-direction (a) and in the y-direction (b). (c) and (d) are the corresponding amplitude profiles along the dashed lines in 2(a) and 2(b), respectively.

Fig. 3.
Fig. 3.

Distributions of the induced third-order polarizations (Py components) in the y-z plane under the excitation polarizations in the y-direction and the scatterers’ orientations along the z-direction (a) and the y-direction (b). Distributions of the induced third-order polarizations (Px components) in the x-y plane under the excitation polarizations in the y-direction and the scatterers’ orientations along the z-direction (c) and the y-direction (d). The corresponding amplitude profiles along the dashed lines in the top panel are displayed in the bottom panel.

Fig. 4.
Fig. 4.

Distributions of the induced polarization component Px in the y-z plane (a); in the x-y plane (b); and the component Py in the x-y plane (c), respectively. The bottom panel shows the corresponding amplitude profiles along the dashed lines indicated in the top panel. Note that the scatterers are oriented along the y-direction while the excitation light polarization is along the x-diection (Fig. 1(d)).

Fig. 5.
Fig. 5.

The induced third-order nonlinear polarizations (Py ) in the y-z plane for nanoparticles with different diameters (a= λp /4; b= 3λp /8; c= λp /2; d= 3λp /4; e=λp ) under the excitation light polarization along the y-direction with the nanoparticles orientated in the z-direction (first panel), and the y-direction (second panel), respectively. The corresponding amplitude profiles along the dashed lines in the first and second panels are displayed in the bottom panel.

Fig. 6.
Fig. 6.

The induced nonlinear polarizations (Px ) in the x-y plane under the excitation light polarization along the y-direction for nanoparticles with different diameters (a= λp /4; b= 3λp /8; c= λp/2; d= 3λp /4; e=λp ) being orientated in the z-direction (first panel), and the y-direction (second panel), respectively. The corresponding amplitude profiles along the dashed lines in the first and second panels are displayed in the bottom panel.

Equations (3)

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{ × H = D t × E = B t
{ E x n + 1 ( i + 0.5 , j , k ) = CA ( r ) · E x n ( i + 0.5 , j , k ) + CB ( r ) [ ( H z n + 0.5 ( i + 0.5 , j + 0.5 , k ) H z n + 0.5 ( i + 0.5 , j 0.5 , k ) ) / Δ y ( H y n + 0.5 ( i + 0.5 , j , k + 0.5 ) H y n + 0.5 ( i + 0.5 , j , k 0.5 ) ) / Δz E y n + 1 ( i , j + 0.5 , k ) = CA ( r ) · E x n ( i , j + 0.5 , k ) + CB ( r ) [ ( H x n + 0.5 ( i , j + 0.5 , k + 0.5 ) H x n + 0.5 ( i , j + 0.5 , k 0.5 ) ) / Δz ( H y n + 0.5 ( i + 0.5 , j + 0.5 , k ) H z n + 0.5 ( i 0.5 , j + 0.5 , k ) ) / Δ x E z n + 1 ( i , j , k + 0.5 ) = CA ( r ) · E x n ( i , j , k + 0.5 ) + CB ( r ) [ ( H y n + 0.5 ( i + 0.5 , j , k + 0.5 ) H y n + 0.5 ( i 0.5 , j , k 0.5 ) ) / Δ x ( H x n + 0.5 ( i + 0.5 , k + 0.5 , k ) H x n + 0.5 ( i , j 0.5 , k + 0.5 ) ) / Δy
P i ( 3 ) ( r , ω as ) = 2 χ ijkl ( 3 ) jkl E j ( r , ω p ) E k ( r , ω p ) E l * ( r , ω s )

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