Abstract

We apply coherent anti-Stokes Raman Scattering (CARS) microscopy to characterize director structures in liquid crystals. We demonstrate that the polarized CARS signal in these anisotropic fluids strongly depends on alignment of chemical bonds/molecules with respect to the collinear polarizations of Stokes and pump/probe excitation beams. This dependence allows for the visualization of the bond/molecular orientations via polarized detection of the CARS signal and thus for CARS polarization microscopy of liquid crystal director fields, as we demonstrate using structures in nematic, cholesteric, and smectic liquid crystals. On the other hand, laser-induced director realignment at powers above a well-defined threshold provides the capability for all-optical CARS signal enhancement in liquid crystals. Moreover, since the liquid crystalline alignment can be controlled by electric and magnetic fields, this demonstrates the feasibility of CARS signal modulation by applying external fields to these materials.

© 2008 Optical Society of America

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    [CrossRef]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
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    [CrossRef] [PubMed]
  43. H. Wang, Y. Fu, and 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]
  44. I. I. Smalyukh, D. S. Kaputa, A. V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Optical trapping of director structures and defects in liquid crystals using laser tweezers," Opt. Express 15, 4359-4371 (2007).
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    [CrossRef]

2007

P. Palffy-Muhoray, "The Diverse World of Liquid Crystals," Phys. Today 60, 54-60 (2007).
[CrossRef]

A.V. Kachynski, A. N. Kuzmin, P. N. Prasad, and I. I. Smalyukh, "Coherent anti-Stokes Raman scattering polarized microscopy of 3-D director structures in liquid crystals," Appl. Phys. Lett. 91, 151905 (2007).
[CrossRef]

B. G. Saar, H.-S. Park, X. S. Xie, and O. D. Lavrentovich, "Three-dimensional imaging of chemical bond orientation in liquid crystals by coherent anti-Stokes Raman scattering microscopy," Opt. Express 15, 13585-13596 (2007).
[CrossRef] [PubMed]

C. D. Southern and H. F. Gleeson, "Using the full Raman depolarization in the determination of the order parameters in liquid crystal systems," Eur. Phys. J. E 24, 119-127 (2007).
[CrossRef] [PubMed]

H. Wang, Y. Fu, and 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]

I. I. Smalyukh, D. S. Kaputa, A. V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Optical trapping of director structures and defects in liquid crystals using laser tweezers," Opt. Express 15, 4359-4371 (2007).
[CrossRef] [PubMed]

I. I. Smalyukh, "Confocal Microscopy of Director Structures in Strongly Confined and Composite Systems," Mol. Cryst. Liq. Cryst. 477, 23-41 (2007).
[CrossRef]

2006

I. I. Smalyukh, O. V. Zribi, J. C. Butler, O. D. Lavrentovich, and G. C. L. Wong, "Structure and Dynamics of Liquid Crystalline Pattern Formation in Drying Droplets of DNA," Phys. Rev. Lett. 96, 177801 (2006).
[CrossRef] [PubMed]

Y. Fu, H. Wang, R. Shi, and J. -X. Cheng, "Characterization of photodamage in coherent anti-Stokes Raman scattering microscopy," Opt. Express 14, 3942-3951 (2006).
[CrossRef] [PubMed]

I. I. Smalyukh, A.V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Laser trapping in anisotropic fluids and polarization controlled particle dynamics," Proc. Nat. Acad. Sci. U.S.A. 103, 18048-18053 (2006).
[CrossRef]

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

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

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Y. Fu, H. Wang, R. Shi, and J.-X. Cheng, "Characterization of photodamage in coherent anti-Stokes Raman scattering microscopy," Opt. Express 14, 3942-3951 (2006).
[CrossRef] [PubMed]

H. Kano and H.-O. Hamaguchi, "In-vivo multi-nonlinear optical imaging of a living cell using a supercontinuum light source generated from a photonic crystal fiber," Opt. Express 14, 2798-2804 (2006).
[CrossRef] [PubMed]

L.G. Rodriguez, S. J. Lockett, and G. R. Holtom, "Coherent anti-Stokes Raman scattering microscopy: a biological review," Cytometry 69A, 779-791 (2006).
[CrossRef]

2005

A. Volkmer, "Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy," J. Phys. D: Appl. Phys. 38, R59-R81 (2005).
[CrossRef]

H. Wang, Y. Fu, P. Zickmund, R. Shi, and J.-X. Cheng, "Coherent Anti-Stokes Raman Scattering Imaging of Axonal Myelin in Live Spinal Tissues," Biophys. J. 89, 581-591 (2005).
[CrossRef] [PubMed]

A. P. Kennedy, J. Sutcliffe, and J.-X. Cheng, "Molecular Composition and Orientation in Myelin figures Characterized by Coherent Anti-Stokes Raman Scattering Microscopy," Langmuir 21, 6478-6486 (2005).
[CrossRef] [PubMed]

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

K. Yoshiki, M. Hashimoto, and T. Araki, "Second-Harmonic-Generation Microscopy Using Excitation Beam with Controlled Polarization Pattern to Determine Three-Dimensional Molecular Orientation," Jpn. J. Appl. Phys. 44, L1066-L1068 (2005).
[CrossRef]

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[CrossRef]

I. I. Smalyukh, R. Pratibha, N. V. Madhusudana, and O. D. Lavrentovich, "Selective imaging of 3-D director fields and study of defects in biaxial smectic A liquid crystals," Eur. Phys. J. E 16, 179-192 (2005).
[CrossRef] [PubMed]

2004

A. Xie and D. A. Higgins, "Electric-field-induced dynamics in radial liquid crystal droplets studied by multiphoton-excited fluorescence microscopy," Appl. Phys. Lett. 84, 4014-4016 (2004).
[CrossRef]

G. W. H. Wurpel, J. M. Schins, and M. Muller, "Direct measurement of chain order in single lipid mono- and bilayers with multiplex CARS," J. Phys. Chem. B 108, 3400-3403 (2004).
[CrossRef]

J.-X. Cheng and S. Xie, "Coherent Anti-Stokes Raman Scattering Microscopy: Instrumentation, Theory, and Applications," J. Phys. Chem. B 108, 827-840 (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]

2003

I. O. Potma and X. S. Xie, "Detection of single lipid bilayers with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Raman Spectrosc. 34, 642-650 (2003).
[CrossRef]

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

S. Pautot, B. J. Frisken, J.-X. Cheng, X. S. Xie, and D. A. Weitz, "Spontaneous Formation of Lipid Structures at Oil/Water/Lipid Interfaces," Langmuir 19, 10281-10287 (2003).
[CrossRef]

D. A. Higgins and B. J. Luther, "Watching molecules reorient in liquid crystal droplets with multiphoton-excited fluorescence microscopy," J. Chem. Phys. 119, 3935-3942 (2003).
[CrossRef]

2001

J.-X. Cheng, L. D. Book, and X. S. Xie, "Polarization coherent anti-Stokes Raman scattering polarized 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

A. 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]

1987

E. Santamato, G. Abbate, P. Maddalena, and Y. R. Shen, "Optically induced twist Freedericksz transition in planar-aligned nematic liquid crystals," Phys. Rev. A 36, 2389-2392 (1987).
[CrossRef] [PubMed]

I.-C. Khoo, P. Y. Yan, and T. H. Liu, "Nonlinear transverse dependence of optically induced director axis reorientation of a nematic liquid crystal film - theory and experiment," J. Opt. Soc. Am. B 4, 115-120 (1987).
[CrossRef]

1982

1981

S. D. Durbin, S. M. Arakelian, and Y. R. Shen, "Optical-field-induced birefringence and Freedericksz transition in a nematic liquid crystal," Phys. Rev. Lett. 47, 1411-1411 (1981).
[CrossRef]

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]

Abbate, G.

E. Santamato, G. Abbate, P. Maddalena, and Y. R. Shen, "Optically induced twist Freedericksz transition in planar-aligned nematic liquid crystals," Phys. Rev. A 36, 2389-2392 (1987).
[CrossRef] [PubMed]

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]

Arakelian, S. M.

S. D. Durbin, S. M. Arakelian, and Y. R. Shen, "Optical-field-induced birefringence and Freedericksz transition in a nematic liquid crystal," Phys. Rev. Lett. 47, 1411-1411 (1981).
[CrossRef]

Araki, T.

K. Yoshiki, M. Hashimoto, and T. Araki, "Second-Harmonic-Generation Microscopy Using Excitation Beam with Controlled Polarization Pattern to Determine Three-Dimensional Molecular Orientation," Jpn. J. Appl. Phys. 44, L1066-L1068 (2005).
[CrossRef]

Beaurepaire, E.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[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," Vibr.Spectroscopy 41, 48-58 (2006).
[CrossRef]

Bodnar, V. H.

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[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," Vibr.Spectroscopy 41, 48-58 (2006).
[CrossRef]

Brakenhoff, C. J.

Butler, J. C.

I. I. Smalyukh, O. V. Zribi, J. C. Butler, O. D. Lavrentovich, and G. C. L. Wong, "Structure and Dynamics of Liquid Crystalline Pattern Formation in Drying Droplets of DNA," Phys. Rev. Lett. 96, 177801 (2006).
[CrossRef] [PubMed]

Cheng, J. X.

Cheng, J. -X.

Cheng, J.-X.

Y. Fu, H. Wang, R. Shi, and J.-X. Cheng, "Characterization of photodamage in coherent anti-Stokes Raman scattering microscopy," Opt. Express 14, 3942-3951 (2006).
[CrossRef] [PubMed]

H. Wang, Y. Fu, P. Zickmund, R. Shi, and J.-X. Cheng, "Coherent Anti-Stokes Raman Scattering Imaging of Axonal Myelin in Live Spinal Tissues," Biophys. J. 89, 581-591 (2005).
[CrossRef] [PubMed]

A. P. Kennedy, J. Sutcliffe, and J.-X. Cheng, "Molecular Composition and Orientation in Myelin figures Characterized by Coherent Anti-Stokes Raman Scattering Microscopy," Langmuir 21, 6478-6486 (2005).
[CrossRef] [PubMed]

J.-X. Cheng and S. Xie, "Coherent Anti-Stokes Raman Scattering Microscopy: Instrumentation, Theory, and Applications," J. Phys. Chem. B 108, 827-840 (2004).
[CrossRef]

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

S. Pautot, B. J. Frisken, J.-X. Cheng, X. S. Xie, and D. A. Weitz, "Spontaneous Formation of Lipid Structures at Oil/Water/Lipid Interfaces," Langmuir 19, 10281-10287 (2003).
[CrossRef]

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

Cicerone, M. T.

Combettes, L.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Débarre, D.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Duncan, M. D.

Durbin, S. D.

S. D. Durbin, S. M. Arakelian, and Y. R. Shen, "Optical-field-induced birefringence and Freedericksz transition in a nematic liquid crystal," Phys. Rev. Lett. 47, 1411-1411 (1981).
[CrossRef]

Fabre, A.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Frisken, B. J.

S. Pautot, B. J. Frisken, J.-X. Cheng, X. S. Xie, and D. A. Weitz, "Spontaneous Formation of Lipid Structures at Oil/Water/Lipid Interfaces," Langmuir 19, 10281-10287 (2003).
[CrossRef]

Fu, Y.

Gartland, E. C.

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[CrossRef]

Gleeson, H. F.

C. D. Southern and H. F. Gleeson, "Using the full Raman depolarization in the determination of the order parameters in liquid crystal systems," Eur. Phys. J. E 24, 119-127 (2007).
[CrossRef] [PubMed]

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]

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.-O.

Hashimoto, M.

K. Yoshiki, M. Hashimoto, and T. Araki, "Second-Harmonic-Generation Microscopy Using Excitation Beam with Controlled Polarization Pattern to Determine Three-Dimensional Molecular Orientation," Jpn. J. Appl. Phys. 44, L1066-L1068 (2005).
[CrossRef]

Higgins, D. A.

A. Xie and D. A. Higgins, "Electric-field-induced dynamics in radial liquid crystal droplets studied by multiphoton-excited fluorescence microscopy," Appl. Phys. Lett. 84, 4014-4016 (2004).
[CrossRef]

D. A. Higgins and B. J. Luther, "Watching molecules reorient in liquid crystal droplets with multiphoton-excited fluorescence microscopy," J. Chem. Phys. 119, 3935-3942 (2003).
[CrossRef]

Holtom, G. R.

L.G. Rodriguez, S. J. Lockett, and G. R. Holtom, "Coherent anti-Stokes Raman scattering microscopy: a biological review," Cytometry 69A, 779-791 (2006).
[CrossRef]

A. 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]

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]

Huang, H.

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[CrossRef]

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]

Kachynski, A. V.

Kachynski, A.V.

A.V. Kachynski, A. N. Kuzmin, P. N. Prasad, and I. I. Smalyukh, "Coherent anti-Stokes Raman scattering polarized microscopy of 3-D director structures in liquid crystals," Appl. Phys. Lett. 91, 151905 (2007).
[CrossRef]

I. I. Smalyukh, A.V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Laser trapping in anisotropic fluids and polarization controlled particle dynamics," Proc. Nat. Acad. Sci. U.S.A. 103, 18048-18053 (2006).
[CrossRef]

Kano, H.

Kaputa, D. S.

Kee, T. W.

Kennedy, A. P.

A. P. Kennedy, J. Sutcliffe, and J.-X. Cheng, "Molecular Composition and Orientation in Myelin figures Characterized by Coherent Anti-Stokes Raman Scattering Microscopy," Langmuir 21, 6478-6486 (2005).
[CrossRef] [PubMed]

Khoo, I.-C.

Kosa, T.

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[CrossRef]

Kuzmin, A. N.

A.V. Kachynski, A. N. Kuzmin, P. N. Prasad, and I. I. Smalyukh, "Coherent anti-Stokes Raman scattering polarized microscopy of 3-D director structures in liquid crystals," Appl. Phys. Lett. 91, 151905 (2007).
[CrossRef]

I. I. Smalyukh, D. S. Kaputa, A. V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Optical trapping of director structures and defects in liquid crystals using laser tweezers," Opt. Express 15, 4359-4371 (2007).
[CrossRef] [PubMed]

I. I. Smalyukh, A.V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Laser trapping in anisotropic fluids and polarization controlled particle dynamics," Proc. Nat. Acad. Sci. U.S.A. 103, 18048-18053 (2006).
[CrossRef]

Lavrentovich, O. D.

B. G. Saar, H.-S. Park, X. S. Xie, and O. D. Lavrentovich, "Three-dimensional imaging of chemical bond orientation in liquid crystals by coherent anti-Stokes Raman scattering microscopy," Opt. Express 15, 13585-13596 (2007).
[CrossRef] [PubMed]

I. I. Smalyukh, O. V. Zribi, J. C. Butler, O. D. Lavrentovich, and G. C. L. Wong, "Structure and Dynamics of Liquid Crystalline Pattern Formation in Drying Droplets of DNA," Phys. Rev. Lett. 96, 177801 (2006).
[CrossRef] [PubMed]

I. I. Smalyukh, R. Pratibha, N. V. Madhusudana, and O. D. Lavrentovich, "Selective imaging of 3-D director fields and study of defects in biaxial smectic A liquid crystals," Eur. Phys. J. E 16, 179-192 (2005).
[CrossRef] [PubMed]

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[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]

Liu, T. H.

Lockett, S. J.

L.G. Rodriguez, S. J. Lockett, and G. R. Holtom, "Coherent anti-Stokes Raman scattering microscopy: a biological review," Cytometry 69A, 779-791 (2006).
[CrossRef]

Luther, B. J.

D. A. Higgins and B. J. Luther, "Watching molecules reorient in liquid crystal droplets with multiphoton-excited fluorescence microscopy," J. Chem. Phys. 119, 3935-3942 (2003).
[CrossRef]

Maddalena, P.

E. Santamato, G. Abbate, P. Maddalena, and Y. R. Shen, "Optically induced twist Freedericksz transition in planar-aligned nematic liquid crystals," Phys. Rev. A 36, 2389-2392 (1987).
[CrossRef] [PubMed]

Madhusudana, N. V.

I. I. Smalyukh, R. Pratibha, N. V. Madhusudana, and O. D. Lavrentovich, "Selective imaging of 3-D director fields and study of defects in biaxial smectic A liquid crystals," Eur. Phys. J. E 16, 179-192 (2005).
[CrossRef] [PubMed]

Maker, P. D.

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]

Manuccia, T. J.

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]

Muller, M.

R. S. Pillai, M. Oh-e, H. Yokoyama, C. J. Brakenhoff, and M. Muller, "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. Muller, "Imaging orientational order and lipid density in multilamellar vesicles with multiplex CARS microscopy," J. Microsc. 218, 37-45 (2005).
[CrossRef] [PubMed]

G. W. H. Wurpel, J. M. Schins, and M. Muller, "Direct measurement of chain order in single lipid mono- and bilayers with multiplex CARS," J. Phys. Chem. B 108, 3400-3403 (2004).
[CrossRef]

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.

Palffy-Muhoray, P.

P. Palffy-Muhoray, "The Diverse World of Liquid Crystals," Phys. Today 60, 54-60 (2007).
[CrossRef]

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[CrossRef]

Park, H.-S.

Pautot, S.

S. Pautot, B. J. Frisken, J.-X. Cheng, X. S. Xie, and D. A. Weitz, "Spontaneous Formation of Lipid Structures at Oil/Water/Lipid Interfaces," Langmuir 19, 10281-10287 (2003).
[CrossRef]

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

Pena, A.-M.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Pillai, R. S.

Potma, I. O.

I. O. Potma and X. S. Xie, "Detection of single lipid bilayers with coherent anti-Stokes Raman scattering (CARS) microscopy," J. Raman Spectrosc. 34, 642-650 (2003).
[CrossRef]

Prasad, P. N.

A.V. Kachynski, A. N. Kuzmin, P. N. Prasad, and I. I. Smalyukh, "Coherent anti-Stokes Raman scattering polarized microscopy of 3-D director structures in liquid crystals," Appl. Phys. Lett. 91, 151905 (2007).
[CrossRef]

I. I. Smalyukh, D. S. Kaputa, A. V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Optical trapping of director structures and defects in liquid crystals using laser tweezers," Opt. Express 15, 4359-4371 (2007).
[CrossRef] [PubMed]

I. I. Smalyukh, A.V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Laser trapping in anisotropic fluids and polarization controlled particle dynamics," Proc. Nat. Acad. Sci. U.S.A. 103, 18048-18053 (2006).
[CrossRef]

Pratibha, R.

I. I. Smalyukh, R. Pratibha, N. V. Madhusudana, and O. D. Lavrentovich, "Selective imaging of 3-D director fields and study of defects in biaxial smectic A liquid crystals," Eur. Phys. J. E 16, 179-192 (2005).
[CrossRef] [PubMed]

Reintjes, J.

Rinia, H. A.

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

Rodriguez, L.G.

L.G. Rodriguez, S. J. Lockett, and G. R. Holtom, "Coherent anti-Stokes Raman scattering microscopy: a biological review," Cytometry 69A, 779-791 (2006).
[CrossRef]

Saar, B. G.

Santamato, E.

E. Santamato, G. Abbate, P. Maddalena, and Y. R. Shen, "Optically induced twist Freedericksz transition in planar-aligned nematic liquid crystals," Phys. Rev. A 36, 2389-2392 (1987).
[CrossRef] [PubMed]

Schanne-Klein, M.-C.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Schins, J. M.

G. W. H. Wurpel, J. M. Schins, and M. Muller, "Direct measurement of chain order in single lipid mono- and bilayers with multiplex CARS," J. Phys. Chem. B 108, 3400-3403 (2004).
[CrossRef]

Senyuk, B. I.

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[CrossRef]

Shen, Y. R.

E. Santamato, G. Abbate, P. Maddalena, and Y. R. Shen, "Optically induced twist Freedericksz transition in planar-aligned nematic liquid crystals," Phys. Rev. A 36, 2389-2392 (1987).
[CrossRef] [PubMed]

S. D. Durbin, S. M. Arakelian, and Y. R. Shen, "Optical-field-induced birefringence and Freedericksz transition in a nematic liquid crystal," Phys. Rev. Lett. 47, 1411-1411 (1981).
[CrossRef]

Shi, R.

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]

Smalyukh, I. I.

A.V. Kachynski, A. N. Kuzmin, P. N. Prasad, and I. I. Smalyukh, "Coherent anti-Stokes Raman scattering polarized microscopy of 3-D director structures in liquid crystals," Appl. Phys. Lett. 91, 151905 (2007).
[CrossRef]

I. I. Smalyukh, D. S. Kaputa, A. V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Optical trapping of director structures and defects in liquid crystals using laser tweezers," Opt. Express 15, 4359-4371 (2007).
[CrossRef] [PubMed]

I. I. Smalyukh, "Confocal Microscopy of Director Structures in Strongly Confined and Composite Systems," Mol. Cryst. Liq. Cryst. 477, 23-41 (2007).
[CrossRef]

I. I. Smalyukh, O. V. Zribi, J. C. Butler, O. D. Lavrentovich, and G. C. L. Wong, "Structure and Dynamics of Liquid Crystalline Pattern Formation in Drying Droplets of DNA," Phys. Rev. Lett. 96, 177801 (2006).
[CrossRef] [PubMed]

I. I. Smalyukh, A.V. Kachynski, A. N. Kuzmin, and P. N. Prasad, "Laser trapping in anisotropic fluids and polarization controlled particle dynamics," Proc. Nat. Acad. Sci. U.S.A. 103, 18048-18053 (2006).
[CrossRef]

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[CrossRef]

I. I. Smalyukh, R. Pratibha, N. V. Madhusudana, and O. D. Lavrentovich, "Selective imaging of 3-D director fields and study of defects in biaxial smectic A liquid crystals," Eur. Phys. J. E 16, 179-192 (2005).
[CrossRef] [PubMed]

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]

Southern, C. D.

C. D. Southern and H. F. Gleeson, "Using the full Raman depolarization in the determination of the order parameters in liquid crystal systems," Eur. Phys. J. E 24, 119-127 (2007).
[CrossRef] [PubMed]

Supatto, W.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Sutcliffe, J.

A. P. Kennedy, J. Sutcliffe, and J.-X. Cheng, "Molecular Composition and Orientation in Myelin figures Characterized by Coherent Anti-Stokes Raman Scattering Microscopy," Langmuir 21, 6478-6486 (2005).
[CrossRef] [PubMed]

Taheri, B.

I. I. Smalyukh, B. I. Senyuk, P. Palffy-Muhoray, O. D. Lavrentovich, H. Huang, E. C. Gartland, Jr., V. H. Bodnar, T. Kosa, and B. Taheri, "Electric-field-induced nematic-cholesteric transition and three-dimensional director structures in homeotropic cells," Phys. Rev. E 72, 061707 (2005).
[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]

Terhune, R. W

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]

Tordjmann, Th.

D. Débarre, W. Supatto, A.-M. Pena, A. Fabre, Th. Tordjmann, L. Combettes, M.-C. Schanne-Klein, and E. Beaurepaire, "Imaging lipid bodies in cells and tissues using third-harmonic generation microscopy," Nature Methods 3, 47-53 (2006).
[CrossRef]

Volkmer, A.

A. Volkmer, "Vibrational imaging and microspectroscopies based on coherent anti-Stokes Raman scattering microscopy," J. Phys. D: Appl. Phys. 38, R59-R81 (2005).
[CrossRef]

Wang, H.

Warenghem, M.

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

Weitz, D. A.

S. Pautot, B. J. Frisken, J.-X. Cheng, X. S. Xie, and D. A. Weitz, "Spontaneous Formation of Lipid Structures at Oil/Water/Lipid Interfaces," Langmuir 19, 10281-10287 (2003).
[CrossRef]

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

Wong, G. C. L.

I. I. Smalyukh, O. V. Zribi, J. C. Butler, O. D. Lavrentovich, and G. C. L. Wong, "Structure and Dynamics of Liquid Crystalline Pattern Formation in Drying Droplets of DNA," Phys. Rev. Lett. 96, 177801 (2006).
[CrossRef] [PubMed]

Wurpel, G. W. H.

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

G. W. H. Wurpel, J. M. Schins, and M. Muller, "Direct measurement of chain order in single lipid mono- and bilayers with multiplex CARS," J. Phys. Chem. B 108, 3400-3403 (2004).
[CrossRef]

Xie, A.

A. Xie and D. A. Higgins, "Electric-field-induced dynamics in radial liquid crystal droplets studied by multiphoton-excited fluorescence microscopy," Appl. Phys. Lett. 84, 4014-4016 (2004).
[CrossRef]

Xie, S.

J.-X. Cheng and S. Xie, "Coherent Anti-Stokes Raman Scattering Microscopy: Instrumentation, Theory, and Applications," J. Phys. Chem. B 108, 827-840 (2004).
[CrossRef]

Xie, X. S.

B. G. Saar, H.-S. Park, X. S. Xie, and O. D. Lavrentovich, "Three-dimensional imaging of chemical bond orientation in liquid crystals by coherent anti-Stokes Raman scattering microscopy," Opt. Express 15, 13585-13596 (2007).
[CrossRef] [PubMed]

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Cytometry

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Supplementary Material (2)

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Figures (11)

Fig. 1.
Fig. 1.

Raman scattering spectra of the studied LC materials. (a) Raman scattering of 8CB for directions parallel and perpendicular to 0 in a planar cell; the inset shows chemical structure of the 8CB molecule. (b) Raman spectra for single-compound LC 5CB (red), nematic mixture E7 (green), and a mixture of nematic AMLC-0010 and chiral additive CB-15 (~1 Wt. %). For clarity, the spectra have been displaced with respect to each other along the “Intensity” axis.

Fig. 2.
Fig. 2.

CARS-PM setup and the principles of CARS imaging. (a) schematics of the experimental setup: ωs and ωp are frequencies of synchronized picosecond Stokes and pump/probe waves, respectively; M1M7 are dichroic dielectric mirrors; O1, O2 -objectives; F1 and F2 are filter wheels which allow for selection of CARS-PM signal within 620-820 nm; P1P6 are polarizers; the XY scanner is based on computer-controlled galvano mirrors; the detectors (photomultiplier tubes) in the E-CARS and F-CARS channels are marked respectively. (b) the energy diagram with the enhanced anti-Stokes Raman scattering signal at w as=2w p-w s obtained when w p-w s=w νib.

Fig. 3.
Fig. 3.

CARS signal (detected within 620-820 nm spectral range) as a function of the beating frequency ωp -ωs around ωvib of the CN-bond of 8CB; the data are obtained for laser polarizations parallel (red) and perpendicular (black) to 0.

Fig. 4.
Fig. 4.

Angular dependence of intensity in CARS-PM and its comparison to that in FCPM. (a) Experimental F-CARS intensity vs. the angle θ between CARS and 0 in uniformly-aligned planar cell with 5CB; the red line shows the expected ICARS ∝cos8 θ dependence. (b) Simultaneously-measured F-CARS and E-CARS signals vs. θ obtained in a planar cell of 8CB; the E-CARS signal is weaker than that of F-CARS even at an increased PMT gain. (c) FCPM intensity vs. the angle between FCPM and in a BTBP-doped nematic LC and the respective theoretical dependence IFCPM (θFCPM )∝cos4 θFCPM (red line).

Fig. 5.
Fig. 5.

Effects of laser-induced realignment on the CARS-PM signal. (a) CARS intensity vs. the scanning area in a homeotropic 5CB sample. Insets in (a) show the observed laser-induced transition from a uniform state (inset ii) to a distorted state (inset i) observed when the area is decreased or power is increased. (b) CARS intensity vs. the incident laser power Wp +Ws for a constant scanning area 7.5µm×7.5µm and for a diffraction-limited spot of ~1µm 2 (inset). (c) CARS intensity vs. WsWp 2 for a scanning area of 7.5µm×7.5µm in homeotropic (CARS 0) and planar (CARS 0) cells. (d) CARS intensity vs. WsW 2 p for a diffraction-limited spot of ~1µm 2 in a homeotropic cell. Experimental points are shown by filled symbols. Red circles and arrows indicate the threshold power per area for the laser-induced transition.

Fig. 6.
Fig. 6.

CARS intensity vs. WsW 2 p for a planar cell with 0 at 0, 20, 45, and 90 degrees to CARS measured for (a) a sample area of 200µm×200µm and (b) a diffraction-limited spot ~1µm 2.

Fig. 7.
Fig. 7.

Computer-simulated layered structure of the FCDs observed in the smectic phase of 8CB: (a) FCD with a hyperbola-ellipse pair of confocal defects; (b) the so-called toric FCD with the ellipse/hyperbola degenerated into the circle/straight line.

Fig. 8.
Fig. 8.

Visualization of the FCD’s 3-D layered structure: (a) experimental and (b) computer-simulated CARS-PM cross-section of in the plane of ellipse; (c, 1.4 MB) video sequence of different 3-D CARS-PM perspective views of the FCD structure. (d) CARS-PM intensity scale. [Media 1]

Fig. 9.
Fig. 9.

(a-c) CARS-PM images of a cholesteric finger structure obtained in a homeotropic cell with the E7-CB15 chiral nematic mixture; (d) reconstructed director structure in the finger’s vertical cross-section containing four nonsingular disclinations lines, of which two are λ 1/2 defects of positive sign (red circles) and the other two λ -1/2 of negative sign (blue circles).

Fig. 10.
Fig. 10.

(a-c) CARS-PM images of an array of axially-symmetric cholesteric domains obtained in a homeotropic cell with the AMLC-0010+CB15 mixture; the red ellipsoids on the inset show areas in which molecular orientations closely match orientation of CARS and correspond to high CARS intensity on the image. (d) schematics of the reconstructed -structure in the domain.

Fig. 11.
Fig. 11.

(a, 2.7 MB) CARS-PM video sequence showing images of a cholesteric sample with a junction of defect structures (marked on the image) in a thick (~50µm) planar cell with the AMLC-0010 +CB15 mixture; (b,c) director structures containing (b)λ 1/2 λ -1/2 pair of nonsingular discinations and (c) a quadrupolar structure of 2(λ 1/2 λ -1/2) defects. The disclinations of positive/negative sign are marked by red/blue circles. [Media 2]

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