Abstract

We employ the finite-difference time-domain (FDTD) technique as a numerical approach to studying the effects of scatterers’ sizes on near-field coherent anti-Stokes Raman scattering (CARS) microscopy under tightly focused radially and linearly polarized light excitations. The FDTD results show that in a uniform medium (water), the full width at half maximum (FWHM) (transverse resolution) of radially polarized near-field CARS (RP-CARS) radiation is approximately 7.7% narrower than that of linearly polarized near-field CARS (LP-CARS) imaging, whereas the depth of focus (DOF) of RP-CARS radiation is 6.5% longer than LP-CARS. However, with the presence of scatterers in the uniform medium, both the FHWM and DOF of near-field RP-CARS radiation become much narrower compared to those of near-field LP-CARS radiation. In addition, the signal to nonresonant background ratio of near-field RP-CARS is significantly improved when the scatterer’s size is larger than a half wavelength of the pump light field. This work suggests that near-field CARS radiations are strongly influenced by the scatterers’ sizes in the medium; and near-field RP-CARS microscopy is superior to the near-field LP-CARS by providing both higher transverse and axial resolutions for three-dimensional molecular imaging of fine structures in biological systems.

©2010 Optical Society of America

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  1. 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]
  2. 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(19), 12076–12087 (2007).
    [Crossref] [PubMed]
  3. F. Lu, W. Zheng, and Z. Huang, “Heterodyne polarization coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. Lett. 92(12), 123901 (2008).
    [Crossref]
  4. 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(2), 728–735 (2006).
    [Crossref] [PubMed]
  5. F. Lu, W. Zheng, C. Sheppard, and Z. Huang, “Interferometric polarization coherent anti-Stokes Raman scattering (IP-CARS) microscopy,” Opt. Lett. 33(6), 602–604 (2008).
    [Crossref] [PubMed]
  6. N. Djaker, D. Gachet, N. Sandeau, P. F. Lenne, and H. Rigneault, “Refractive effects in coherent anti-Stokes Raman scattering microscopy,” Appl. Opt. 45(27), 7005–7011 (2006).
    [Crossref] [PubMed]
  7. C. Liu, Z. Huang, F. Lu, W. Zheng, D. W. Hutmacher, and C. Sheppard, “Near-field effects on coherent anti-Stokes Raman scattering microscopy imaging,” Opt. Express 15(7), 4118–4131 (2007).
    [Crossref] [PubMed]
  8. V. V. Krishnamachari and E. O. Potma, “Focus-engineered coherent anti-Stokes Raman scattering microscopy: a numerical investigation,” J. Opt. Soc. Am. A 24(4), 1138–1147 (2007).
    [Crossref]
  9. J. Lin, H. Wang, W. Zheng, F. Lu, C. Sheppard, and Z. Huang, “Numerical study of effects of light polarization, scatterer sizes and orientations on near-field coherent anti-Stokes Raman scattering microscopy,” Opt. Express 17(4), 2423–2434 (2009).
    [Crossref] [PubMed]
  10. H. Wang, L. Shi, B. Lukyanchuk, C. Sheppard, and C. T. Chong, “Creation of a needle of longitudinally polarized light in vacuum using binary optics,” Nat. Photonics 2(8), 501–505 (2008).
    [Crossref]
  11. F. Lu, W. Zheng, and Z. Huang, “Coherent anti-Stokes Raman scattering microscopy using tightly focused radially polarized light,” Opt. Lett. 34(12), 1870–1872 (2009).
    [Crossref] [PubMed]
  12. R. Dorn, S. Quabis, and G. Leuchs, “Sharper focus for a radially polarized light beam,” Phys. Rev. Lett. 91(23), 233901 (2003).
    [Crossref] [PubMed]
  13. L. Novotny, M. R. Beversluis, K. S. Youngworth, and T. G. Brown, “Longitudinal field modes probed by single molecules,” Phys. Rev. Lett. 86(23), 5251–5254 (2001).
    [Crossref] [PubMed]
  14. K. Yoshiki, K. Ryosuke, M. Hashimoto, T. Araki, and N. Hashimoto, “Second-harmonic-generation microscope using eight-segment polarization-mode converter to observe three-dimensional molecular orientation,” Opt. Lett. 32(12), 1680–1682 (2007).
    [Crossref] [PubMed]
  15. S. Yang and Q. Zhan, “Third-harmonic generation microscopy with tightly focused radial polarization,” J. Opt. A, Pure Appl. Opt. 10(12), 125103 (2008).
    [Crossref]
  16. J. X. Cheng and X. S. Xie, “Green’s function formulation for third-harmonic generation microscopy,” J. Opt. Soc. Am. B 19(7), 1604–1610 (2002).
    [Crossref]
  17. 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(14), 143109 (2006).
    [Crossref]
  18. K. S. Yee, “Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media,” IEEE Trans. Antenn. Propag. 14(3), 302–307 (1966).
    [Crossref]
  19. A. Volkmer, “Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy,” J. Phys. D Appl. Phys. 38(5), R59–R81 (2005).
    [Crossref]
  20. 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(1), 27–32 (1992).
    [Crossref]
  21. B. Richards and E. Wolf, “Electromagnetic diffraction in optical systems. II. Structure of the image field in an aplanatic system,” Proc. R. Soc. Lond. A Math. Phys. Sci. 253(1274), 358–379 (1959).
    [Crossref]
  22. D. Courjon and C. Bainier, “Near field microscopy and near field optics,” Rep. Prog. Phys. 57(10), 989–1028 (1994).
    [Crossref]
  23. 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(13), 131110 (2005).
    [Crossref]
  24. 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(34), 8489–8492 (2002).
    [Crossref]
  25. S. Kawata, Y. Inouye, and T. Ichimura, “Near-field optics and spectroscopy for molecular nano-imaging,” Sci. Prog. 87(1), 25–49 (2004).
    [Crossref]

2009 (2)

2008 (4)

H. Wang, L. Shi, B. Lukyanchuk, C. Sheppard, and C. T. Chong, “Creation of a needle of longitudinally polarized light in vacuum using binary optics,” Nat. Photonics 2(8), 501–505 (2008).
[Crossref]

S. Yang and Q. Zhan, “Third-harmonic generation microscopy with tightly focused radial polarization,” J. Opt. A, Pure Appl. Opt. 10(12), 125103 (2008).
[Crossref]

F. Lu, W. Zheng, and Z. Huang, “Heterodyne polarization coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. Lett. 92(12), 123901 (2008).
[Crossref]

F. Lu, W. Zheng, C. Sheppard, and Z. Huang, “Interferometric polarization coherent anti-Stokes Raman scattering (IP-CARS) microscopy,” Opt. Lett. 33(6), 602–604 (2008).
[Crossref] [PubMed]

2007 (4)

2006 (3)

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(2), 728–735 (2006).
[Crossref] [PubMed]

N. Djaker, D. Gachet, N. Sandeau, P. F. Lenne, and H. Rigneault, “Refractive effects in coherent anti-Stokes Raman scattering microscopy,” Appl. Opt. 45(27), 7005–7011 (2006).
[Crossref] [PubMed]

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(14), 143109 (2006).
[Crossref]

2005 (2)

A. Volkmer, “Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy,” J. Phys. D Appl. Phys. 38(5), R59–R81 (2005).
[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(13), 131110 (2005).
[Crossref]

2004 (1)

S. Kawata, Y. Inouye, and T. Ichimura, “Near-field optics and spectroscopy for molecular nano-imaging,” Sci. Prog. 87(1), 25–49 (2004).
[Crossref]

2003 (1)

R. Dorn, S. Quabis, and G. Leuchs, “Sharper focus for a radially polarized light beam,” Phys. Rev. Lett. 91(23), 233901 (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(7), 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(34), 8489–8492 (2002).
[Crossref]

2001 (1)

L. Novotny, M. R. Beversluis, K. S. Youngworth, and T. G. Brown, “Longitudinal field modes probed by single molecules,” Phys. Rev. Lett. 86(23), 5251–5254 (2001).
[Crossref] [PubMed]

1999 (1)

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]

1994 (1)

D. Courjon and C. Bainier, “Near field microscopy and near field optics,” Rep. Prog. Phys. 57(10), 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(1), 27–32 (1992).
[Crossref]

1966 (1)

K. S. Yee, “Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media,” IEEE Trans. Antenn. Propag. 14(3), 302–307 (1966).
[Crossref]

1959 (1)

B. Richards and E. Wolf, “Electromagnetic diffraction in optical systems. II. Structure of the image field in an aplanatic system,” Proc. R. Soc. Lond. A Math. Phys. Sci. 253(1274), 358–379 (1959).
[Crossref]

Araki, T.

Bainier, C.

D. Courjon and C. Bainier, “Near field microscopy and near field optics,” Rep. Prog. Phys. 57(10), 989–1028 (1994).
[Crossref]

Beversluis, M. R.

L. Novotny, M. R. Beversluis, K. S. Youngworth, and T. G. Brown, “Longitudinal field modes probed by single molecules,” Phys. Rev. Lett. 86(23), 5251–5254 (2001).
[Crossref] [PubMed]

Brown, T. G.

L. Novotny, M. R. Beversluis, K. S. Youngworth, and T. G. Brown, “Longitudinal field modes probed by single molecules,” Phys. Rev. Lett. 86(23), 5251–5254 (2001).
[Crossref] [PubMed]

Cheng, J. X.

Chong, C. T.

H. Wang, L. Shi, B. Lukyanchuk, C. Sheppard, and C. T. Chong, “Creation of a needle of longitudinally polarized light in vacuum using binary optics,” Nat. Photonics 2(8), 501–505 (2008).
[Crossref]

Courjon, D.

D. Courjon and C. Bainier, “Near field microscopy and near field optics,” Rep. Prog. Phys. 57(10), 989–1028 (1994).
[Crossref]

Djaker, N.

Dorn, R.

R. Dorn, S. Quabis, and G. Leuchs, “Sharper focus for a radially polarized light beam,” Phys. Rev. Lett. 91(23), 233901 (2003).
[Crossref] [PubMed]

Evans, C. L.

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(13), 131110 (2005).
[Crossref]

Gu, M.

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(13), 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(34), 8489–8492 (2002).
[Crossref]

Hashimoto, M.

Hashimoto, N.

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(14), 143109 (2006).
[Crossref]

Holtom, G. R.

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]

Huang, Z.

Hutmacher, D. W.

Ichimura, T.

S. Kawata, Y. Inouye, and T. Ichimura, “Near-field optics and spectroscopy for molecular nano-imaging,” Sci. Prog. 87(1), 25–49 (2004).
[Crossref]

Inouye, Y.

S. Kawata, Y. Inouye, and T. Ichimura, “Near-field optics and spectroscopy for molecular nano-imaging,” Sci. Prog. 87(1), 25–49 (2004).
[Crossref]

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(1), 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(14), 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(13), 131110 (2005).
[Crossref]

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(14), 143109 (2006).
[Crossref]

S. Kawata, Y. Inouye, and T. Ichimura, “Near-field optics and spectroscopy for molecular nano-imaging,” Sci. Prog. 87(1), 25–49 (2004).
[Crossref]

Kesari, S.

Krishnamachari, V. V.

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(34), 8489–8492 (2002).
[Crossref]

Lenne, P. F.

Leuchs, G.

R. Dorn, S. Quabis, and G. Leuchs, “Sharper focus for a radially polarized light beam,” Phys. Rev. Lett. 91(23), 233901 (2003).
[Crossref] [PubMed]

Lin, J.

Liu, C.

Lu, F.

Lukyanchuk, B.

H. Wang, L. Shi, B. Lukyanchuk, C. Sheppard, and C. T. Chong, “Creation of a needle of longitudinally polarized light in vacuum using binary optics,” Nat. Photonics 2(8), 501–505 (2008).
[Crossref]

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(14), 143109 (2006).
[Crossref]

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(1), 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(2), 728–735 (2006).
[Crossref] [PubMed]

Novotny, L.

L. Novotny, M. R. Beversluis, K. S. Youngworth, and T. G. Brown, “Longitudinal field modes probed by single molecules,” Phys. Rev. Lett. 86(23), 5251–5254 (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(4), 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(2), 728–735 (2006).
[Crossref] [PubMed]

Quabis, S.

R. Dorn, S. Quabis, and G. Leuchs, “Sharper focus for a radially polarized light beam,” Phys. Rev. Lett. 91(23), 233901 (2003).
[Crossref] [PubMed]

Richards, B.

B. Richards and E. Wolf, “Electromagnetic diffraction in optical systems. II. Structure of the image field in an aplanatic system,” Proc. R. Soc. Lond. A Math. Phys. Sci. 253(1274), 358–379 (1959).
[Crossref]

Rigneault, H.

Ryosuke, K.

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(14), 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(34), 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(34), 8489–8492 (2002).
[Crossref]

Sheppard, C.

Shi, L.

H. Wang, L. Shi, B. Lukyanchuk, C. Sheppard, and C. T. Chong, “Creation of a needle of longitudinally polarized light in vacuum using binary optics,” Nat. Photonics 2(8), 501–505 (2008).
[Crossref]

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(1), 27–32 (1992).
[Crossref]

Volkmer, A.

A. Volkmer, “Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy,” J. Phys. D Appl. Phys. 38(5), R59–R81 (2005).
[Crossref]

Wang, H.

J. Lin, H. Wang, W. Zheng, F. Lu, C. Sheppard, and Z. Huang, “Numerical study of effects of light polarization, scatterer sizes and orientations on near-field coherent anti-Stokes Raman scattering microscopy,” Opt. Express 17(4), 2423–2434 (2009).
[Crossref] [PubMed]

H. Wang, L. Shi, B. Lukyanchuk, C. Sheppard, and C. T. Chong, “Creation of a needle of longitudinally polarized light in vacuum using binary optics,” Nat. Photonics 2(8), 501–505 (2008).
[Crossref]

Wolf, E.

B. Richards and E. Wolf, “Electromagnetic diffraction in optical systems. II. Structure of the image field in an aplanatic system,” Proc. R. Soc. Lond. A Math. Phys. Sci. 253(1274), 358–379 (1959).
[Crossref]

Wong, S. T. C.

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(19), 12076–12087 (2007).
[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(2), 728–735 (2006).
[Crossref] [PubMed]

J. X. Cheng and X. S. Xie, “Green’s function formulation for third-harmonic generation microscopy,” J. Opt. Soc. Am. B 19(7), 1604–1610 (2002).
[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]

Xu, X.

Yang, S.

S. Yang and Q. Zhan, “Third-harmonic generation microscopy with tightly focused radial polarization,” J. Opt. A, Pure Appl. Opt. 10(12), 125103 (2008).
[Crossref]

Yee, K. S.

K. S. Yee, “Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media,” IEEE Trans. Antenn. Propag. 14(3), 302–307 (1966).
[Crossref]

Yoshiki, K.

Young, G. S.

Youngworth, K. S.

L. Novotny, M. R. Beversluis, K. S. Youngworth, and T. G. Brown, “Longitudinal field modes probed by single molecules,” Phys. Rev. Lett. 86(23), 5251–5254 (2001).
[Crossref] [PubMed]

Zhan, Q.

S. Yang and Q. Zhan, “Third-harmonic generation microscopy with tightly focused radial polarization,” J. Opt. A, Pure Appl. Opt. 10(12), 125103 (2008).
[Crossref]

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(34), 8489–8492 (2002).
[Crossref]

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. 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(14), 143109 (2006).
[Crossref]

F. Lu, W. Zheng, and Z. Huang, “Heterodyne polarization coherent anti-Stokes Raman scattering microscopy,” Appl. Phys. Lett. 92(12), 123901 (2008).
[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(13), 131110 (2005).
[Crossref]

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(2), 728–735 (2006).
[Crossref] [PubMed]

IEEE Trans. Antenn. Propag. (1)

K. S. Yee, “Numerical solution of initial boundary value problem involving Maxwell equations in isotropic media,” IEEE Trans. Antenn. Propag. 14(3), 302–307 (1966).
[Crossref]

J. Opt. A, Pure Appl. Opt. (1)

S. Yang and Q. Zhan, “Third-harmonic generation microscopy with tightly focused radial polarization,” J. Opt. A, Pure Appl. Opt. 10(12), 125103 (2008).
[Crossref]

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

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

J. Phys. Chem. B (1)

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(34), 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(5), R59–R81 (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(1), 27–32 (1992).
[Crossref]

Nat. Photonics (1)

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Figures (5)

Fig. 1
Fig. 1 Schematic of near-field LP-CARS or RP-CARS field (ECARS) generation under tightly focused linearly polarized (e.g., y-polarized) or radially polarized pump (Ep) and Stokes (Es) light fields through a high NA objective. LP-CARS, linearly polarized CARS; RP-CARS, radially polarized CARS. The calculation volume was divided into cubic cells of λp/40 at each step, where λp (750 nm) is the pump beam wavelength, and the wavelength of Stokes beam λs is chosen to be 852 nm, and then the generated CARS signal is at 670 nm, representing a resonant Raman shift of 1600 cm−1 of mono-substituted benzene rings stretching vibrations in polystyrene beads [19]. The refractive indices of the scatterer (polystyrene beads) and surrounding medium (water) are assumed to be 1.59 and 1.33, respectively [20].

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Fig. 2
Fig. 2 Comparison of near-field CARS intensity distributions in the y-z plane between the RP-CARS (z-component) (a) and the LP-CARS (y-component) (b) generated from pure water. Comparison of the intensity profiles of RP-CARS and LP-CARS in the lateral (c) and axial (d) directions along the corresponding lines indicated in Figs. 2(a) and 2(b).

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Fig. 3
Fig. 3 Near-field intensity distributions of RP-CARS and LP-CARS for scatterers with diameters of (a) 0.1λp; (b) 0.25λp; (c) 0.5λp; (d) 0.75λp; and (e) 1.0λp, respectively. The first and third panels represent the intensity distributions in the y-z plane for RP-CARS and LP-CARS, respectively. The corresponding intensity profiles along the white lines in the first and third panels of Fig. 3 are plotted in the second and fourth panels, respectively.

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Fig. 4
Fig. 4 The full width at half maximum (FWHM) (a) and the depth of focus (DOF) (b) of RP-CARS and LP-CARS with water alone, and with water and scatterers in different sizes (D = 0.1λp, 0.25λp, 0.5λp, 0.75, and 1.0λp). Note that the values at zero scatterer’s size means the scattering medium is pure water.

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Fig. 5
Fig. 5 Comparison of signal to background ratios (SBR) of RP-CARS and LP-CARS versus scatterers’ sizes (D = 0.1λp, 0.25λp, 0.5λp, 0.75, and 1.0λp).

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Equations (6)

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E(ρ,φ,z)=−iA[I0+I2cos2φI2sin2φ2I1cosφ],
In=∫0αe−sin2θ/sin2αsinθcos1/2(θ)gn(θ)Jn(kρsinθ)eikzcosθdθ,
Ez(ρ,z)=2iA∫0αcos1/2(θ)sin2(θ)l(θ)J0(kρsinθ)eikzcosθdθ,
Eρ(ρ,z)=2A∫0αcos1/2(θ)sin(2θ)l(θ)J1(kρsinθ)eikzcosθdθ,
l(θ)=exp[−β02(sinθcosα)2]J1(2β0sinθsinα),
Pi(3)(r,ωas)=3∑jklχijkl(3)Ej(r,ωp)Ek(r,ωp)El*(r,ωs),

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