Abstract

Coherent anti-Stokes Raman scattering (CARS) microscopy is demonstrated to be a promising optical method for the characterization of polymer films with film thickness varying between 180 nm to 4300 nm. In case of PMMA films with a thickness of few hundreds of nanometers, the observed CARS signal was mainly associated with the interference effect of large nonresonant CARS field from glass substrate and the weak resonant field of PMMA. The dependence of resonant CARS intensity of PMMA film on film thickness is in good agreement with the theoretical prediction on a CARS field. The current work offers potential possibilities of noninvasive thickness measurement of polymeric thin film of thickness less than 180 nm by multiplex CARS microscopy without depth-profiling.

© 2008 Optical Society of America

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  1. G. Hougham, G. Tesoro, and J. Shaw, "Synthesis and properties of highly fluorinated polyimides," Macromolecules 27, 3642-3649 (1994).
    [CrossRef]
  2. J. Canning, "Potentials and challenges for lithography beyond 193 nm optics," J. Vac. Sci. Technol. B 15,2109-2111 (1997).
    [CrossRef]
  3. Jerome P. Silverman, "X-ray lithography: status, challenges, and outlook for 0.13 ?m," J. Vac. Sci. Technol. B 15. 2117-2124 (1997).
    [CrossRef]
  4. Mark A. McCord, "Electron beam lithography for 0.13 ?m manufacturing," J. Vac. Sci. Technol. B 15, 2125-2129 (1997).
    [CrossRef]
  5. Lioyd R. Harriott, "Scattering with angular limitation projection electron beam lithography for suboptical lithography," J. Vac. Sci. Technol. B 15,2130-2135 (1997).
    [CrossRef]
  6. G. Gross, "Ion projection lithography: next generation technology," J. Vac. Sci. Technol. B 15,2136-2139 (1997).
    [CrossRef]
  7. J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
    [CrossRef]
  8. H.K. Kim, F.G. Shi, B. Zao, and M. R. Brongo, "Thickness-dependent optical and dielectric behaviors of low-k polymer thin films," In Proc. SPIE 4181, 114-120 (2000).
    [CrossRef]
  9. K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
    [CrossRef]
  10. R. Ohmura, S. Kashiwazaki, and Y. H. Mori, "Measurements of clathrate-hydrate film thickness using laser interferometry," J. Crystal Growth 218, 72-380 (2000).
    [CrossRef]
  11. C. Jung and B. K. Rhee, "Simultaneous determination of thickness and optical constants of polymer thin film by analyzing transmittance," Appl. Opt. 41, 3861-3865 (2002).
    [CrossRef] [PubMed]
  12. R. Wang and P. L. Wong, "Optical characteristics of thin film coating and measurement of its thickness," Trib. Trans. 30, 801-806 (1997).
  13. B. P. Bunt, "Measurement of thickness of thin transparent films using fluorescence," British J. Appl. Phys. 12, 175-177 (1961).
    [CrossRef]
  14. H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
    [CrossRef]
  15. P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
    [CrossRef]
  16. M. Muller, and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106, 3715-3723 (2002).
    [CrossRef]
  17. B. Dragnea, J. Preusser, W. Schade, and S. R. Leone, "Transmission near-field scanning microscope for infrared chemical imaging," J. Appl. Phys. 86, 2795-2799 (1999).
    [CrossRef]
  18. Ligia Muntean and Romain Planques, A. L. D. Kilcoyne, Stephen R. Leone, Mary K. Gilles, and William D. Hinsberg, "Chemical mapping of polymer photoresists by scanning transmission x-ray microscopy," J. Vac. Sci. Technol. B 23,1630-1636 (2005).
    [CrossRef]
  19. P. D. Maker and R. W. Terhune, "Study of optical effects due to an induced polarization third order in the electric field strength," Phys. Rev. 137, A801-A818 (1965).
    [CrossRef]
  20. A. C. Eckbreth, Laser diagnostics for combustion temperature and species, (Abacus Press, Prunbridge Wells, 1988).
  21. M. D. Duncan, J. Reintjes, and T. J. Manuccia, "Scanning coherent anti-stokes Raman microscope," Opt. Lett. 7, 350-352 (1982).
    [CrossRef] [PubMed]
  22. Zumbusch, 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]
  23. Ji-Xin Cheng, A. Volkmer, and X. S. Xie, "Theoretical and experimental characterization of coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 19, 1363-1375 (2002).
    [CrossRef]
  24. E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
    [CrossRef]
  25. B. V. Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blends imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectroscopy 38, 916-926 (2007).
    [CrossRef]
  26. H. Kano and H. Hamaguchi, "Femtosecond coherent anti-stokes Raman scattering spectroscopy using a supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85, 4298-4300 (2004).
    [CrossRef]
  27. T. W. Kee and M. T. Cicerone, "Simple approach to one-laser, broadband coherent anti-stokes Raman scattering microscopy," Opt. Lett. 29, 2701-2703 (2004).
    [CrossRef] [PubMed]
  28. H. Wang, Y. Fu, nd J. X. Cheng, "Experimental observation and theoretical analysis of Raman resonance-enhanced photodamage in coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 24, 544-552 (2007).
    [CrossRef]
  29. M. A. Seo and D. S. Kim, H. S. Kim, D. S. Choi, and S. C. Jeoung, "Formation of photoluminescent germanium nanostructures by femtosecond laser processing on bulk germanium: role of ambient gases," Opt. Express 14, 4908 (2006).
    [CrossRef] [PubMed]
  30. J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
    [CrossRef]
  31. G. Vignaud, J.-F. Bardeau, A. Gibaud, and Y. Grohens, "Multiple glass-transition temperatures in thin supported films of isotactic PMMA as revealed by enhanced Raman scattering," Langmuir 21, 8601-8604 (2005).
    [CrossRef] [PubMed]

2007 (2)

B. V. Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blends imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectroscopy 38, 916-926 (2007).
[CrossRef]

H. Wang, Y. Fu, nd J. X. Cheng, "Experimental observation and theoretical analysis of Raman resonance-enhanced photodamage in coherent anti-Stokes Raman scattering microscopy," J. Opt. Soc. Am. B 24, 544-552 (2007).
[CrossRef]

2006 (2)

M. A. Seo and D. S. Kim, H. S. Kim, D. S. Choi, and S. C. Jeoung, "Formation of photoluminescent germanium nanostructures by femtosecond laser processing on bulk germanium: role of ambient gases," Opt. Express 14, 4908 (2006).
[CrossRef] [PubMed]

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

2005 (2)

G. Vignaud, J.-F. Bardeau, A. Gibaud, and Y. Grohens, "Multiple glass-transition temperatures in thin supported films of isotactic PMMA as revealed by enhanced Raman scattering," Langmuir 21, 8601-8604 (2005).
[CrossRef] [PubMed]

Ligia Muntean and Romain Planques, A. L. D. Kilcoyne, Stephen R. Leone, Mary K. Gilles, and William D. Hinsberg, "Chemical mapping of polymer photoresists by scanning transmission x-ray microscopy," J. Vac. Sci. Technol. B 23,1630-1636 (2005).
[CrossRef]

2004 (4)

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-stokes Raman scattering spectroscopy using a supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85, 4298-4300 (2004).
[CrossRef]

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

T. W. Kee and M. T. Cicerone, "Simple approach to one-laser, broadband coherent anti-stokes Raman scattering microscopy," Opt. Lett. 29, 2701-2703 (2004).
[CrossRef] [PubMed]

2002 (3)

2000 (3)

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

H.K. Kim, F.G. Shi, B. Zao, and M. R. Brongo, "Thickness-dependent optical and dielectric behaviors of low-k polymer thin films," In Proc. SPIE 4181, 114-120 (2000).
[CrossRef]

R. Ohmura, S. Kashiwazaki, and Y. H. Mori, "Measurements of clathrate-hydrate film thickness using laser interferometry," J. Crystal Growth 218, 72-380 (2000).
[CrossRef]

1999 (2)

B. Dragnea, J. Preusser, W. Schade, and S. R. Leone, "Transmission near-field scanning microscope for infrared chemical imaging," J. Appl. Phys. 86, 2795-2799 (1999).
[CrossRef]

Zumbusch, 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]

1998 (1)

P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
[CrossRef]

1997 (6)

R. Wang and P. L. Wong, "Optical characteristics of thin film coating and measurement of its thickness," Trib. Trans. 30, 801-806 (1997).

J. Canning, "Potentials and challenges for lithography beyond 193 nm optics," J. Vac. Sci. Technol. B 15,2109-2111 (1997).
[CrossRef]

Jerome P. Silverman, "X-ray lithography: status, challenges, and outlook for 0.13 ?m," J. Vac. Sci. Technol. B 15. 2117-2124 (1997).
[CrossRef]

Mark A. McCord, "Electron beam lithography for 0.13 ?m manufacturing," J. Vac. Sci. Technol. B 15, 2125-2129 (1997).
[CrossRef]

Lioyd R. Harriott, "Scattering with angular limitation projection electron beam lithography for suboptical lithography," J. Vac. Sci. Technol. B 15,2130-2135 (1997).
[CrossRef]

G. Gross, "Ion projection lithography: next generation technology," J. Vac. Sci. Technol. B 15,2136-2139 (1997).
[CrossRef]

1996 (1)

H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
[CrossRef]

1994 (1)

G. Hougham, G. Tesoro, and J. Shaw, "Synthesis and properties of highly fluorinated polyimides," Macromolecules 27, 3642-3649 (1994).
[CrossRef]

1982 (1)

1965 (1)

P. D. Maker and R. W. Terhune, "Study of optical effects due to an induced polarization third order in the electric field strength," Phys. Rev. 137, A801-A818 (1965).
[CrossRef]

1961 (1)

B. P. Bunt, "Measurement of thickness of thin transparent films using fluorescence," British J. Appl. Phys. 12, 175-177 (1961).
[CrossRef]

Asada, K.

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

Bardeau, J.-F.

G. Vignaud, J.-F. Bardeau, A. Gibaud, and Y. Grohens, "Multiple glass-transition temperatures in thin supported films of isotactic PMMA as revealed by enhanced Raman scattering," Langmuir 21, 8601-8604 (2005).
[CrossRef] [PubMed]

Boccara, A. C.

H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
[CrossRef]

Brongo, M. R.

H.K. Kim, F.G. Shi, B. Zao, and M. R. Brongo, "Thickness-dependent optical and dielectric behaviors of low-k polymer thin films," In Proc. SPIE 4181, 114-120 (2000).
[CrossRef]

Brongo, M.R.

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

Bunt, B. P.

B. P. Bunt, "Measurement of thickness of thin transparent films using fluorescence," British J. Appl. Phys. 12, 175-177 (1961).
[CrossRef]

Byers, J.

P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
[CrossRef]

Canning, J.

J. Canning, "Potentials and challenges for lithography beyond 193 nm optics," J. Vac. Sci. Technol. B 15,2109-2111 (1997).
[CrossRef]

Cella, N.

H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
[CrossRef]

Chao, K.

P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
[CrossRef]

Cho, B. R.

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

Choi, D. S.

Cicerone, M. T.

Dragnea, B.

B. Dragnea, J. Preusser, W. Schade, and S. R. Leone, "Transmission near-field scanning microscope for infrared chemical imaging," J. Appl. Phys. 86, 2795-2799 (1999).
[CrossRef]

Duncan, M. D.

Fu, Y.

Gibaud, A.

G. Vignaud, J.-F. Bardeau, A. Gibaud, and Y. Grohens, "Multiple glass-transition temperatures in thin supported films of isotactic PMMA as revealed by enhanced Raman scattering," Langmuir 21, 8601-8604 (2005).
[CrossRef] [PubMed]

Grohens, Y.

G. Vignaud, J.-F. Bardeau, A. Gibaud, and Y. Grohens, "Multiple glass-transition temperatures in thin supported films of isotactic PMMA as revealed by enhanced Raman scattering," Langmuir 21, 8601-8604 (2005).
[CrossRef] [PubMed]

Gross, G.

G. Gross, "Ion projection lithography: next generation technology," J. Vac. Sci. Technol. B 15,2136-2139 (1997).
[CrossRef]

Hamaguchi, H.

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-stokes Raman scattering spectroscopy using a supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85, 4298-4300 (2004).
[CrossRef]

Harriott, Lioyd R.

Lioyd R. Harriott, "Scattering with angular limitation projection electron beam lithography for suboptical lithography," J. Vac. Sci. Technol. B 15,2130-2135 (1997).
[CrossRef]

Hinsberg, W. D.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Hougham, G.

G. Hougham, G. Tesoro, and J. Shaw, "Synthesis and properties of highly fluorinated polyimides," Macromolecules 27, 3642-3649 (1994).
[CrossRef]

Ishikawa, K.

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

Iwata, K.

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

Jeon, S. J.

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

Jeoung, S. C.

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

M. A. Seo and D. S. Kim, H. S. Kim, D. S. Choi, and S. C. Jeoung, "Formation of photoluminescent germanium nanostructures by femtosecond laser processing on bulk germanium: role of ambient gases," Opt. Express 14, 4908 (2006).
[CrossRef] [PubMed]

Ji-Xin Cheng,

Jones, D.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Jung, C.

Kagawa, K.

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

Kano, H.

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-stokes Raman scattering spectroscopy using a supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85, 4298-4300 (2004).
[CrossRef]

Kashiwazaki, S.

R. Ohmura, S. Kashiwazaki, and Y. H. Mori, "Measurements of clathrate-hydrate film thickness using laser interferometry," J. Crystal Growth 218, 72-380 (2000).
[CrossRef]

Kee, T. W.

Kim, C. H.

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

Kim, D. S.

Kim, H. M.

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

Kim, H. S.

Kim, H.K.

H.K. Kim, F.G. Shi, B. Zao, and M. R. Brongo, "Thickness-dependent optical and dielectric behaviors of low-k polymer thin films," In Proc. SPIE 4181, 114-120 (2000).
[CrossRef]

Leone, S. R.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

B. Dragnea, J. Preusser, W. Schade, and S. R. Leone, "Transmission near-field scanning microscope for infrared chemical imaging," J. Appl. Phys. 86, 2795-2799 (1999).
[CrossRef]

Lim, K.S.

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

Maker, P. D.

P. D. Maker and R. W. Terhune, "Study of optical effects due to an induced polarization third order in the electric field strength," Phys. Rev. 137, A801-A818 (1965).
[CrossRef]

Manuccia, T. J.

McCord, Mark A.

Mark A. McCord, "Electron beam lithography for 0.13 ?m manufacturing," J. Vac. Sci. Technol. B 15, 2125-2129 (1997).
[CrossRef]

Mendenhall, J.

P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
[CrossRef]

Meyer, L.

B. V. Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blends imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectroscopy 38, 916-926 (2007).
[CrossRef]

Mori, Y. H.

R. Ohmura, S. Kashiwazaki, and Y. H. Mori, "Measurements of clathrate-hydrate film thickness using laser interferometry," J. Crystal Growth 218, 72-380 (2000).
[CrossRef]

Motzkus, M.

B. V. Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blends imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectroscopy 38, 916-926 (2007).
[CrossRef]

Muller, M.

M. Muller, and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106, 3715-3723 (2002).
[CrossRef]

Muntean, L.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Nam, J. L.

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

Nieh, T.G.

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

Ohmura, R.

R. Ohmura, S. Kashiwazaki, and Y. H. Mori, "Measurements of clathrate-hydrate film thickness using laser interferometry," J. Crystal Growth 218, 72-380 (2000).
[CrossRef]

Potma, E. O.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Preusser, J.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

B. Dragnea, J. Preusser, W. Schade, and S. R. Leone, "Transmission near-field scanning microscope for infrared chemical imaging," J. Appl. Phys. 86, 2795-2799 (1999).
[CrossRef]

Qu, S.

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

Reintjes, J.

Rhee, B. K.

Rhleb, H. E.

H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
[CrossRef]

Roger, J. P.

H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
[CrossRef]

Rosenmayer, T.

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

Schade, W.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

B. Dragnea, J. Preusser, W. Schade, and S. R. Leone, "Transmission near-field scanning microscope for infrared chemical imaging," J. Appl. Phys. 86, 2795-2799 (1999).
[CrossRef]

Schins, J. M.

M. Muller, and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106, 3715-3723 (2002).
[CrossRef]

Seo, M. A.

Shaw, J.

G. Hougham, G. Tesoro, and J. Shaw, "Synthesis and properties of highly fluorinated polyimides," Macromolecules 27, 3642-3649 (1994).
[CrossRef]

Shi, F.G.

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

H.K. Kim, F.G. Shi, B. Zao, and M. R. Brongo, "Thickness-dependent optical and dielectric behaviors of low-k polymer thin films," In Proc. SPIE 4181, 114-120 (2000).
[CrossRef]

Silverman, Jerome P.

Jerome P. Silverman, "X-ray lithography: status, challenges, and outlook for 0.13 ?m," J. Vac. Sci. Technol. B 15. 2117-2124 (1997).
[CrossRef]

Terhune, R. W.

P. D. Maker and R. W. Terhune, "Study of optical effects due to an induced polarization third order in the electric field strength," Phys. Rev. 137, A801-A818 (1965).
[CrossRef]

Tesoro, G.

G. Hougham, G. Tesoro, and J. Shaw, "Synthesis and properties of highly fluorinated polyimides," Macromolecules 27, 3642-3649 (1994).
[CrossRef]

Ueda, M.

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

Vacano, B. V.

B. V. Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blends imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectroscopy 38, 916-926 (2007).
[CrossRef]

Vignaud, G.

G. Vignaud, J.-F. Bardeau, A. Gibaud, and Y. Grohens, "Multiple glass-transition temperatures in thin supported films of isotactic PMMA as revealed by enhanced Raman scattering," Langmuir 21, 8601-8604 (2005).
[CrossRef] [PubMed]

Wang, H.

Wang, J.

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

Wang, R.

R. Wang and P. L. Wong, "Optical characteristics of thin film coating and measurement of its thickness," Trib. Trans. 30, 801-806 (1997).

Webber, S. E.

P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
[CrossRef]

Wong, P. L.

R. Wang and P. L. Wong, "Optical characteristics of thin film coating and measurement of its thickness," Trib. Trans. 30, 801-806 (1997).

Xie, X. S.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Yamano, H.

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

Ye, J.

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Zao, B.

H.K. Kim, F.G. Shi, B. Zao, and M. R. Brongo, "Thickness-dependent optical and dielectric behaviors of low-k polymer thin films," In Proc. SPIE 4181, 114-120 (2000).
[CrossRef]

Zhang, P. L.

P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
[CrossRef]

Zhao, B.

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

Zuber, A.

H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
[CrossRef]

Zumbusch,

Zumbusch, 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. (1)

H. Kano and H. Hamaguchi, "Femtosecond coherent anti-stokes Raman scattering spectroscopy using a supercontinuum generated from a photonic crystal fiber," Appl. Phys. Lett. 85, 4298-4300 (2004).
[CrossRef]

British J. Appl. Phys. (1)

B. P. Bunt, "Measurement of thickness of thin transparent films using fluorescence," British J. Appl. Phys. 12, 175-177 (1961).
[CrossRef]

Chem. Phys. Lett. (1)

J. L. Nam, C. H. Kim, S. C. Jeoung, K.S. Lim, H. M. Kim, S. J. Jeon, B. R. Cho, "Measurement of two-photon absorption coefficient of dye molecules doped in polymer thin films based on ultrafast laser ablation," Chem. Phys. Lett. 427, 210-214 (2006)
[CrossRef]

In Proc. SPIE (2)

P. L. Zhang, S. E. Webber, J. Mendenhall, J. Byers, and K. Chao, "Diffusion of photoacid generators by laser scanning confocal microscopy," In Proc. SPIE 3333, 794-805(1998).
[CrossRef]

H.K. Kim, F.G. Shi, B. Zao, and M. R. Brongo, "Thickness-dependent optical and dielectric behaviors of low-k polymer thin films," In Proc. SPIE 4181, 114-120 (2000).
[CrossRef]

J. Appl. Phys. (1)

B. Dragnea, J. Preusser, W. Schade, and S. R. Leone, "Transmission near-field scanning microscope for infrared chemical imaging," J. Appl. Phys. 86, 2795-2799 (1999).
[CrossRef]

J. Crystal Growth (1)

R. Ohmura, S. Kashiwazaki, and Y. H. Mori, "Measurements of clathrate-hydrate film thickness using laser interferometry," J. Crystal Growth 218, 72-380 (2000).
[CrossRef]

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

J. Phys. Chem. B (2)

E. O. Potma, X. S. Xie, L. Muntean, J. Preusser, D. Jones, J. Ye, S. R. Leone, W. D. Hinsberg, and W. Schade, "Chemical imaging of phtoresists with coherent anti-stokes Raman scattering microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

M. Muller, and J. M. Schins, "Imaging the thermodynamic state of lipid membranes with multiplex CARS microscopy," J. Phys. Chem. B 106, 3715-3723 (2002).
[CrossRef]

J. Raman Spectroscopy (1)

B. V. Vacano, L. Meyer, and M. Motzkus, "Rapid polymer blends imaging with quantitative broadband multiplex CARS microscopy," J. Raman Spectroscopy 38, 916-926 (2007).
[CrossRef]

J. Vac. Sci. Technol. B (6)

Ligia Muntean and Romain Planques, A. L. D. Kilcoyne, Stephen R. Leone, Mary K. Gilles, and William D. Hinsberg, "Chemical mapping of polymer photoresists by scanning transmission x-ray microscopy," J. Vac. Sci. Technol. B 23,1630-1636 (2005).
[CrossRef]

J. Canning, "Potentials and challenges for lithography beyond 193 nm optics," J. Vac. Sci. Technol. B 15,2109-2111 (1997).
[CrossRef]

Jerome P. Silverman, "X-ray lithography: status, challenges, and outlook for 0.13 ?m," J. Vac. Sci. Technol. B 15. 2117-2124 (1997).
[CrossRef]

Mark A. McCord, "Electron beam lithography for 0.13 ?m manufacturing," J. Vac. Sci. Technol. B 15, 2125-2129 (1997).
[CrossRef]

Lioyd R. Harriott, "Scattering with angular limitation projection electron beam lithography for suboptical lithography," J. Vac. Sci. Technol. B 15,2130-2135 (1997).
[CrossRef]

G. Gross, "Ion projection lithography: next generation technology," J. Vac. Sci. Technol. B 15,2136-2139 (1997).
[CrossRef]

Langmuir (1)

G. Vignaud, J.-F. Bardeau, A. Gibaud, and Y. Grohens, "Multiple glass-transition temperatures in thin supported films of isotactic PMMA as revealed by enhanced Raman scattering," Langmuir 21, 8601-8604 (2005).
[CrossRef] [PubMed]

Macromolecules (1)

G. Hougham, G. Tesoro, and J. Shaw, "Synthesis and properties of highly fluorinated polyimides," Macromolecules 27, 3642-3649 (1994).
[CrossRef]

Opt. Express (1)

Opt. Laser Eng. (1)

K. Ishikawa, H. Yamano, K. Kagawa, K. Asada, K. Iwata, and M. Ueda, "Measurement of thickness of a thin film by means of laser interference at many incident angles," Opt. Laser Eng. 41, 19-29 (2004).
[CrossRef]

Opt. Lett. (2)

Phys. Rev. (1)

P. D. Maker and R. W. Terhune, "Study of optical effects due to an induced polarization third order in the electric field strength," Phys. Rev. 137, A801-A818 (1965).
[CrossRef]

Phys. Rev. Lett. (1)

Zumbusch, 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]

Scr. Mater. (1)

J. Wang, F.G. Shi, T.G. Nieh, B. Zhao, M.R. Brongo, S. Qu, and T. Rosenmayer, " Thickness dependence of elastic modulus and hardness of on-wafer low-k ultrathin polytetrafluoroethylene films," Scr. Mater. 42, 687-694 (2000).
[CrossRef]

Thin Solid Films (1)

H. E. Rhleb, N. Cella, J. P. Roger, A. C. Boccara, and A. Zuber, "Beam size and collimation effects in spectroscopic ellipsometry of transparent films with optical thickness inhomogeneity," Thin Solid Films 288, 125-131 (1996).
[CrossRef]

Trib. Trans. (1)

R. Wang and P. L. Wong, "Optical characteristics of thin film coating and measurement of its thickness," Trib. Trans. 30, 801-806 (1997).

Other (1)

A. C. Eckbreth, Laser diagnostics for combustion temperature and species, (Abacus Press, Prunbridge Wells, 1988).

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Figures (6)

Fig.1.
Fig.1.

Experimental setup of multiplex CARS microscopy for characterization of polymeric thin films.

Fig.2.
Fig.2.

PMMA film thickness as a function of repeated number of coatings. The inset shows cross sectional profile of the ablated surface of PMMA thin film with 1500 nm in thickness. The thickness was determined by measuring the height difference between the intact surface of PMMA and the bare glass substrate.

Fig. 3.
Fig. 3.

Multiplex CARS (a) and cw-Raman spectral features (b) of PMMA thin films coated on a slide glass substrate. Raman peaks at 2842 cm-1, 2932 cm-1, 2952 cm-1, 3000 cm-1, and 3058 cm-1 are in good agreement with reported values [15]. (c-g) are the selected CARS spectral features of PMMA films with a thickness of 180 nm, 715 nm, 1310 nm, 2070 nm, and 4300 nm, respectively. The experimental observation was denoted with black circle. The red solid lines are the best spectra resulted from the fitting procedure of the observed spectra with Eq (3-6) (see text).

Fig. 4.
Fig. 4.

CARS intensity as a function of the thickness of the PMMA film. The experimental observation was denoted with black circle. Blue circles are the resonant CARS signal from PMMA film resulted from the fitting procedure of the observed spectra with Eq (3-6) (see text). Red solid line represents the dependence of resonant CARS signal resulted from theoretical consideration of CARS field scattered from PMMA disk. For comparison, the line with a slope of two was also displayed by green dotted line.

Fig. 5.
Fig. 5.

Radiation pattern of far-field CARS from PMMA disk (n=1.5). CARS scatters was centered at the tight focus with high numerical aperture (NA=0.9) with various thickness.

Fig. 6.
Fig. 6.

Multiplex CARS intensity profile (blue solid circles) along axial direction for about 870 nm thick film of PMMA coated on slide glass (a). The intensity profile of resonant CARS signal from PMMA (black solid circles) was fitted by Gaussian function. Full width at half maximum was found to be ca. 2.1 um (red solid line). (b-f) represents specificity of depth profile at several depth positions. The experimental observation was denoted with black circle. The red (blue, green, magenta) solid lines are the best results from total (PMMA, cross term, only glass) spectral fitting using Eq. (3).

Equations (7)

Equations on this page are rendered with MathJax. Learn more.

I 3 = ω a s 2 n 1 2 n 2 n 3 c 4 ε 0 2 I 1 2 I 2 χ C A R S 2 l 2 sinc 2 ( Δ k l 2 )
I CARS ( ω as ) χ CARS ( 3 ) ( ω as ) 2 = i χ r , i ( 3 ) + χ nr ( 3 ) 2
χ C A R S ( 3 ) 2 = i χ P M M A , r , i ( 3 ) + χ P M M A , n r ( 3 ) 2 + 2 · χ G l a s s , n r ( 3 )
× R e { i χ P M M A , r , i ( 3 ) + χ P M M A , n r ( 3 ) } + χ G l a s s , n r ( 3 ) 2
χ P M M A , r , i ( 3 ) = A i Ω i ( ω p ω s ) i Γ i
χ P M M A , n r ( 3 ) = B · exp ( 2 ( ω ω c ) 2 ln 2 Δ c 2 )
χ g l a s s , n r ( 3 ) = C · exp ( 2 ( ω ω c ) 2 ln 2 Δ c 2 )

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