Abstract

Liquid crystals are a class of industrially important materials whose optical properties make them useful particularly in display technology. Optical imaging of these materials provides information about their structure and physical properties. Coherent anti-Stokes Raman scattering (CARS) microscopy is used to provide three-dimensional chemical maps of liquid crystalline samples without the use of external labels. CARS is an optical imaging technique that derives contrast from Raman-active molecular vibrations in the sample. Compared to many other three-dimensional imaging techniques, CARS offers more rapid chemical characterization without the use of external dyes or contrast agents. The use of CARS to image chemical and orientational order in liquid crystals is demonstrated using several examples, and the limitations and benefits are discussed.

© 2007 Optical Society of America

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  16. 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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  17. T. B. Huff, and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
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    [CrossRef]
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  20. H. Kano and H. Hamaguchi, "Three-dimensional vibrational imaging of a microcrystalline J-aggregate using supercontinuum-based ultra-broadband multiplex coherent cnti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 3120-3126 (2006).
    [CrossRef] [PubMed]
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    [CrossRef]
  27. E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
    [CrossRef]
  28. J.-X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
    [CrossRef]

2007

K. Kaznacheev and T. Hegmann, "Molecular ordering in biaxial smectic-A phase studied by scanning transmission X-ray microscopy (STXM)," Phys. Chem. Chem. Phys. 9, 1705-1712 (2007).
[CrossRef] [PubMed]

P. Camorani, and M. P. Fontana, "Local three-dimensional characterization of a micro-patterned liquid crystalline cell by confocal Raman microscopy," Mol. Cryst. Liq. Cryst. 465, 143 - 152 (2007).
[CrossRef]

T. B. Huff, and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

2006

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]

H. Kano and H. Hamaguchi, "Three-dimensional vibrational imaging of a microcrystalline J-aggregate using supercontinuum-based ultra-broadband multiplex coherent cnti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 3120-3126 (2006).
[CrossRef] [PubMed]

G. W. H. Wurpel and M. Müller, "Water confined by lipid bilayers: A multiplex CARS study," Chem. Phys. Lett. 425, 336-341 (2006).
[CrossRef]

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

J. F. Blach, M. Warenghem, and D. Bormann, "Probing thick uniaxial birefringent medium in confined geometry: A polarised confocal micro-Raman approach," Vib. Spectrosc. 41, 48-58 (2006).
[CrossRef]

R. S. Pillai, M. Oh-e, H. Yokoyama, G. J. Brakenhoff, and M. Müller, "Imaging colloidal particle induced topological defects in a nematic liquid crystal using third harmonic generation microscopy," Opt. Express 14, 12976-12983 (2006).
[CrossRef] [PubMed]

2005

G. W. H. Wurpel, H. A. Rinia, and M. Müller, "Imaging orientational order and lipid density in multilamellar vesicles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (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. USA 102, 16807-16812 (2005).
[CrossRef]

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

2004

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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

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

2002

W. J. Jones, D. K. Thomas, D. W. Thomas, and G. Williams. "Raman scattering studies of homogenous and twisted-nematic liquid crystal cells and the determination of ?P2? and ?P4? order parameters." J. Mol. Struct. 614, 75-85, (2002).
[CrossRef]

2001

J.-X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
[CrossRef]

I. I. Smalyukh, S. V. Shiyanovskii, and O. D. Lavrentovich, "Three-dimensional imaging of orientational order by fluorescence confocal polarizing microscopy," Chem. Phys. Lett. 336, 88-96 (2001).
[CrossRef]

1999

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Phase-Matched Third-Harmonic Generation in a Nematic Liquid Crystal Cell," Phys. Rev. Lett. 82, 3046 (1999).
[CrossRef]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy," Appl. Phys. Lett. 74, 3107-3109 (1999).
[CrossRef]

1997

W. J. Jones, "Picosecond inverse Raman spectroscopy of liquid crystals," J. Mol. Struct. 404, 129-136 (1997).
[CrossRef]

1990

J. R. Bellare, H. T. Davis, W. G. Miller, and L. E. Scriven, "Polarized Optical Microscopy of Anisotropic Media: Imaging, Theory and Simulations," J. Colloid Interface Sci. 136, 305-326 (1990).
[CrossRef]

Akagi, K.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Astrova, E. V.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Barad, Y.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy," Appl. Phys. Lett. 74, 3107-3109 (1999).
[CrossRef]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Phase-Matched Third-Harmonic Generation in a Nematic Liquid Crystal Cell," Phys. Rev. Lett. 82, 3046 (1999).
[CrossRef]

Bellare, J. R.

J. R. Bellare, H. T. Davis, W. G. Miller, and L. E. Scriven, "Polarized Optical Microscopy of Anisotropic Media: Imaging, Theory and Simulations," J. Colloid Interface Sci. 136, 305-326 (1990).
[CrossRef]

Blach, J. F.

J. F. Blach, M. Warenghem, and D. Bormann, "Probing thick uniaxial birefringent medium in confined geometry: A polarised confocal micro-Raman approach," Vib. Spectrosc. 41, 48-58 (2006).
[CrossRef]

Book, L. D.

Bormann, D.

J. F. Blach, M. Warenghem, and D. Bormann, "Probing thick uniaxial birefringent medium in confined geometry: A polarised confocal micro-Raman approach," Vib. Spectrosc. 41, 48-58 (2006).
[CrossRef]

Brakenhoff, G. J.

Budagovsky, I. A.

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

Camorani, P.

P. Camorani, and M. P. Fontana, "Local three-dimensional characterization of a micro-patterned liquid crystalline cell by confocal Raman microscopy," Mol. Cryst. Liq. Cryst. 465, 143 - 152 (2007).
[CrossRef]

Cheng, J. X.

T. B. Huff, and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

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

Cheng, J.-X.

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

Davis, H. T.

J. R. Bellare, H. T. Davis, W. G. Miller, and L. E. Scriven, "Polarized Optical Microscopy of Anisotropic Media: Imaging, Theory and Simulations," J. Colloid Interface Sci. 136, 305-326 (1990).
[CrossRef]

Enikeeva, V. A.

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

Evans, C. L.

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

Fontana, M. P.

P. Camorani, and M. P. Fontana, "Local three-dimensional characterization of a micro-patterned liquid crystalline cell by confocal Raman microscopy," Mol. Cryst. Liq. Cryst. 465, 143 - 152 (2007).
[CrossRef]

Goh, M.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Grudinkin, S. A.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Guo, S.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Hamaguchi, H.

H. Kano and H. Hamaguchi, "Three-dimensional vibrational imaging of a microcrystalline J-aggregate using supercontinuum-based ultra-broadband multiplex coherent cnti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 3120-3126 (2006).
[CrossRef] [PubMed]

Hegmann, T.

K. Kaznacheev and T. Hegmann, "Molecular ordering in biaxial smectic-A phase studied by scanning transmission X-ray microscopy (STXM)," Phys. Chem. Chem. Phys. 9, 1705-1712 (2007).
[CrossRef] [PubMed]

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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Houkawa, Y.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Huff, T. B.

T. B. Huff, and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

Ishikawa, K.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Jones, W. J.

W. J. Jones, D. K. Thomas, D. W. Thomas, and G. Williams. "Raman scattering studies of homogenous and twisted-nematic liquid crystal cells and the determination of ?P2? and ?P4? order parameters." J. Mol. Struct. 614, 75-85, (2002).
[CrossRef]

W. J. Jones, "Picosecond inverse Raman spectroscopy of liquid crystals," J. Mol. Struct. 404, 129-136 (1997).
[CrossRef]

Kano, H.

H. Kano and H. Hamaguchi, "Three-dimensional vibrational imaging of a microcrystalline J-aggregate using supercontinuum-based ultra-broadband multiplex coherent cnti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 3120-3126 (2006).
[CrossRef] [PubMed]

Kaznacheev, K.

K. Kaznacheev and T. Hegmann, "Molecular ordering in biaxial smectic-A phase studied by scanning transmission X-ray microscopy (STXM)," Phys. Chem. Chem. Phys. 9, 1705-1712 (2007).
[CrossRef] [PubMed]

Kitaeva, V. F.

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

Lavrentovich, O. D.

I. I. Smalyukh, S. V. Shiyanovskii, and O. D. Lavrentovich, "Three-dimensional imaging of orientational order by fluorescence confocal polarizing microscopy," Chem. Phys. Lett. 336, 88-96 (2001).
[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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

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

Makarov, V. A.

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

Miller, W. G.

J. R. Bellare, H. T. Davis, W. G. Miller, and L. E. Scriven, "Polarized Optical Microscopy of Anisotropic Media: Imaging, Theory and Simulations," J. Colloid Interface Sci. 136, 305-326 (1990).
[CrossRef]

Mori, T.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Müller, M.

G. W. H. Wurpel and M. Müller, "Water confined by lipid bilayers: A multiplex CARS study," Chem. Phys. Lett. 425, 336-341 (2006).
[CrossRef]

R. S. Pillai, M. Oh-e, H. Yokoyama, G. J. Brakenhoff, and M. Müller, "Imaging colloidal particle induced topological defects in a nematic liquid crystal using third harmonic generation microscopy," Opt. Express 14, 12976-12983 (2006).
[CrossRef] [PubMed]

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

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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[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]

Ofuji, M.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Oh-e, M.

Ozheredov, I. A.

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

Patel, J. S.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Phase-Matched Third-Harmonic Generation in a Nematic Liquid Crystal Cell," Phys. Rev. Lett. 82, 3046 (1999).
[CrossRef]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy," Appl. Phys. Lett. 74, 3107-3109 (1999).
[CrossRef]

Perova, T. S.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Pillai, R. S.

Pilyugina, Y. A.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Potma, E. O.

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. USA 102, 16807-16812 (2005).
[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 photoresists with coherent anti-Stokes Raman scattering (CARS) 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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Puoris'haag, M.

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

Rinia, H. A.

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

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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Scriven, L. E.

J. R. Bellare, H. T. Davis, W. G. Miller, and L. E. Scriven, "Polarized Optical Microscopy of Anisotropic Media: Imaging, Theory and Simulations," J. Colloid Interface Sci. 136, 305-326 (1990).
[CrossRef]

Shiyanovskii, S. V.

I. I. Smalyukh, S. V. Shiyanovskii, and O. D. Lavrentovich, "Three-dimensional imaging of orientational order by fluorescence confocal polarizing microscopy," Chem. Phys. Lett. 336, 88-96 (2001).
[CrossRef]

Shkurinov, A. P.

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

Silberberg, Y.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Phase-Matched Third-Harmonic Generation in a Nematic Liquid Crystal Cell," Phys. Rev. Lett. 82, 3046 (1999).
[CrossRef]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy," Appl. Phys. Lett. 74, 3107-3109 (1999).
[CrossRef]

Smalyukh, I. I.

I. I. Smalyukh, S. V. Shiyanovskii, and O. D. Lavrentovich, "Three-dimensional imaging of orientational order by fluorescence confocal polarizing microscopy," Chem. Phys. Lett. 336, 88-96 (2001).
[CrossRef]

Takanishi, Y.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Takano, Y.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Takezoe, H.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Thomas, D. K.

W. J. Jones, D. K. Thomas, D. W. Thomas, and G. Williams. "Raman scattering studies of homogenous and twisted-nematic liquid crystal cells and the determination of ?P2? and ?P4? order parameters." J. Mol. Struct. 614, 75-85, (2002).
[CrossRef]

Thomas, D. W.

W. J. Jones, D. K. Thomas, D. W. Thomas, and G. Williams. "Raman scattering studies of homogenous and twisted-nematic liquid crystal cells and the determination of ?P2? and ?P4? order parameters." J. Mol. Struct. 614, 75-85, (2002).
[CrossRef]

Tolmachev, V. A.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Viji, J. K.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Voronkov, V. B.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Warenghem, M.

J. F. Blach, M. Warenghem, and D. Bormann, "Probing thick uniaxial birefringent medium in confined geometry: A polarised confocal micro-Raman approach," Vib. Spectrosc. 41, 48-58 (2006).
[CrossRef]

Williams, G.

W. J. Jones, D. K. Thomas, D. W. Thomas, and G. Williams. "Raman scattering studies of homogenous and twisted-nematic liquid crystal cells and the determination of ?P2? and ?P4? order parameters." J. Mol. Struct. 614, 75-85, (2002).
[CrossRef]

Wurpel, G. W. H.

G. W. H. Wurpel and M. Müller, "Water confined by lipid bilayers: A multiplex CARS study," Chem. Phys. Lett. 425, 336-341 (2006).
[CrossRef]

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

Xie, X. S.

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

J. X. Cheng and X. S. Xie, "Coherent anti-Stokes Raman scattering microscopy: instrumentation, theory, and applications," J. Phys. Chem. B 108, 827-840 (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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

J.-X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering microscopy," Opt. Lett. 26, 1341-1343 (2001).
[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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

Yelin, D.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy," Appl. Phys. Lett. 74, 3107-3109 (1999).
[CrossRef]

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Phase-Matched Third-Harmonic Generation in a Nematic Liquid Crystal Cell," Phys. Rev. Lett. 82, 3046 (1999).
[CrossRef]

Yokoyama, H.

Appl. Phys. Lett.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Depth-resolved imaging of nematic liquid crystals by third-harmonic microscopy," Appl. Phys. Lett. 74, 3107-3109 (1999).
[CrossRef]

Biophys. J.

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]

Chem. Phys. Lett.

I. I. Smalyukh, S. V. Shiyanovskii, and O. D. Lavrentovich, "Three-dimensional imaging of orientational order by fluorescence confocal polarizing microscopy," Chem. Phys. Lett. 336, 88-96 (2001).
[CrossRef]

G. W. H. Wurpel and M. Müller, "Water confined by lipid bilayers: A multiplex CARS study," Chem. Phys. Lett. 425, 336-341 (2006).
[CrossRef]

J. Colloid Interface Sci.

J. R. Bellare, H. T. Davis, W. G. Miller, and L. E. Scriven, "Polarized Optical Microscopy of Anisotropic Media: Imaging, Theory and Simulations," J. Colloid Interface Sci. 136, 305-326 (1990).
[CrossRef]

J. Microsc.

T. B. Huff, and J. X. Cheng, "In vivo coherent anti-Stokes Raman scattering imaging of sciatic nerve tissue," J. Microsc. 225, 175-182 (2007).
[CrossRef] [PubMed]

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

J. Mol. Struct.

W. J. Jones, "Picosecond inverse Raman spectroscopy of liquid crystals," J. Mol. Struct. 404, 129-136 (1997).
[CrossRef]

W. J. Jones, D. K. Thomas, D. W. Thomas, and G. Williams. "Raman scattering studies of homogenous and twisted-nematic liquid crystal cells and the determination of ?P2? and ?P4? order parameters." J. Mol. Struct. 614, 75-85, (2002).
[CrossRef]

J. Phys. Chem. B

H. Kano and H. Hamaguchi, "Three-dimensional vibrational imaging of a microcrystalline J-aggregate using supercontinuum-based ultra-broadband multiplex coherent cnti-Stokes Raman scattering microscopy," J. Phys. Chem. B 110, 3120-3126 (2006).
[CrossRef] [PubMed]

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 photoresists with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Phys. Chem. B 108, 1296-1301 (2004).
[CrossRef]

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

Jpn. J. Appl. Phys.

M. Ofuji, Y. Takano, Y. Houkawa, Y. Takanishi, K. Ishikawa, H. Takezoe, T. Mori, M. Goh, S. Guo, and K. Akagi, "Microscopic orientational order of polymer chains in helical polyacetylene thin films studied by confocal laser Raman microscopy," Jpn. J. Appl. Phys. 45, 1710-1713 (2006).
[CrossRef]

Mol. Cryst. Liq. Cryst.

P. Camorani, and M. P. Fontana, "Local three-dimensional characterization of a micro-patterned liquid crystalline cell by confocal Raman microscopy," Mol. Cryst. Liq. Cryst. 465, 143 - 152 (2007).
[CrossRef]

V. A. Enikeeva, V. A. Makarov, I. A. Ozheredov, A. P. Shkurinov, I. A. Budagovsky, V. F. Kitaeva, Zolot, apos, A. S. ko, and M. I. Barnik, "Orienting influence of femtosecond pulses on nematic liquid crystals," Mol. Cryst. Liq. Cryst. 442, 1 - 18 (2005).
[CrossRef]

Opt. Express

Opt. Lett.

Phys. Chem. Chem. Phys.

K. Kaznacheev and T. Hegmann, "Molecular ordering in biaxial smectic-A phase studied by scanning transmission X-ray microscopy (STXM)," Phys. Chem. Chem. Phys. 9, 1705-1712 (2007).
[CrossRef] [PubMed]

Phys. Rev. Lett.

D. Yelin, Y. Silberberg, Y. Barad, and J. S. Patel, "Phase-Matched Third-Harmonic Generation in a Nematic Liquid Crystal Cell," Phys. Rev. Lett. 82, 3046 (1999).
[CrossRef]

Proc. Natl. Acad. Sci. USA

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

Semiconductors.

E. V. Astrova, T. S. Perova, S. A. Grudinkin, V. A. Tolmachev, Y. A. Pilyugina, V. B. Voronkov, and J. K. Viji, "Polarized infrared and Raman spectroscopic studies of the liquid crystal E7 alignment in composites based on grooved silicon." Semiconductors. 39, 759-767, (2005).
[CrossRef]

Vib. Spectrosc.

J. F. Blach, M. Warenghem, and D. Bormann, "Probing thick uniaxial birefringent medium in confined geometry: A polarised confocal micro-Raman approach," Vib. Spectrosc. 41, 48-58 (2006).
[CrossRef]

Other

E. A. Buyuktanir, K. Zhang, A. Gericke, and J. L. West, "Raman mapping of the orientation of nematic and smectic liquid crystals," in 21st International Liquid Crystal Conference (Keystone, CO, 2006), pp. DFCTP-25.

M. Kleman, and O. D. Lavrentovich, Soft Matter Physics: An Introduction (Springer, New York, 2003).

N. H. Hartshorn, The Microscopy of Liquid Crystals (Microscope Publications, London, 1974).

J. M. Haudin, in Optical Properties of Polymers, G. H. Meeten, ed., (Elsevier, Essex, 1986).

L. M. Blinov, and V. G. Chigrinov, Electrooptic Effects in Liquid Crystal Materials (Springer, New York, 1994).
[CrossRef]

I.-C. Khoo, Liquid Crystals: Physical Properties and Nonlinear Optical Phenomena (Wiley-Interscience, New Jersey, 1994).

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Figures (5)

Fig. 1.
Fig. 1.

CARS Microscopy of Liquid Crystals (a) Energy diagram for coherent anti-Stokes Raman scattering microscopy (b) Schematic of the CARS microscope. Nd:YVO4: 1064 & 532 nm laser; OPO: optical parametric oscillator. DM: dichroic mirror; SU: microscope scan unit; OL: 1.2NA water X60 objective lens; C: 0.55 NA air condenser; PMT: photomultipler tube. (c) Raman spectrum of the E7 liquid crystal, displaying strong peaks at 1600 cm-1 and 2215 cm-1. (d) Chemical composition of the E7 mixture.

Fig. 2.
Fig. 2.

Visualizing the Fredericks transition with CARS (a) CARS signal intensity over time, with the polarization at 45° to the director axis. No change in intensity is seen even at 64 mW average power, demonstrating that we do not optically re-orient the N sample. (b) Calculated average director angle as a function of Z-position for a 20 μm thick E7 cell, at various applied voltages. (c) CARS depth profiles of the E7 cell tuned into the cyano stretch at 2215 cm-1 at various voltages. The loss of signal in the center of the sample at elevated voltages is characteristic of a Frederiks transition, and demonstrates that the cyano groups (and the director) reorient vertically. (d) CARS images of the same sample at the alkyl stretching frequency of 2845 cm-1. Different contrast and much less structure is observed, consistent with the fact that the CH groups are on average perpendicular to the director and associated with the flexible aliphatic chains in E7 molecules.

Fig. 3.
Fig. 3.

CARS images of a Schlieren texture (a)-(d) Images at the aryl stretch at 1600 cm-1, with the excitation beams polarized along the direction indicated by the double-headed arrow. All scale bars are 20 μm. (e) sketch of the director field around a point defect (marked by a circle), based on data from (a)-(d). (f) CARS image at the cyano stretching band at 2215 cm-1 at the indicated polarization. (g) CARS image off resonance, showing minimal contrast at the same detector gain as in (a)-(d) and (f). (h) CARS depth profile along the Z axis taken down the line indicated in (b). X scale bar is 20 μm, Z is 5 μm.

Fig. 4.
Fig. 4.

Smectic texture imaged with CARS. Images are acquired of a smectic liquid crystal at the indicated vibrational difference frequency, with (a,d) cyano at 2215, (b,e) off resonance at 2257 and (c,f) alkyl at 2845 cm-1. The scale bar is 20 μm in each image, and the polarization is along the direction indicated by the double-headed arrow. We observe a strong polarization dependence in the FCDs, with the strongest contrast in these images occurring at the cyano stretching region. Consistent with our results in Fig. 2, we observe less polarization dependence in the CH stretching region.

Fig. 5.
Fig. 5.

Orientation map of the SmA liquid crystal. The background image shown in false color is a map of the polarization of the sample calculated according to (Ix-Iy)/(Ix+Iy) using the images from Figs. 4(a) and 4(d). The overlaid vectors are obtained by smoothing the image using a 9 pixel × 9 pixel moving average and then calculating the polarization angle and magnitude as described in the text. Vectors with polarization magnitude<0.02 are not plotted for clarity. The majority of the vectors in the glycerol portion (bottom half) are therefore not plotted because the medium is isotropic.

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