Graphene recently emerged as a new two-dimensional material platform with unique optical, thermal and electronic properties. Single- or few-atom-thick graphene flakes can potentially be utilized to form structured bulk composites that further enrich these properties and enable a broad range of new applications. Here we describe optical manipulation of self-aligned colloidal graphene flakes in thermotropic liquid crystals of nematic and cholesteric types. Three-dimensional rotational and translational manipulation of graphene flakes by means of holographic optical tweezers allows for non-contact spatial patterning of graphene, control of liquid crystal defects, and low-power optical realignment of the liquid crystal director using these flakes. Potential applications include optically- and electrically-controlled reconfigurable liquid crystalline dispersions of spontaneously aligning colloidal graphene flakes and new electro-optic devices with graphene-based interconnected transparent electrodes at surfaces and in the bulk of liquid crystals.

© 2013 OSA

1. P. Poulin, H. Stark, T. C. Lubensky, and D. A. Weitz, “Novel colloidal interactions in anisotropic fluids,” Science275(5307), 1770–1773 (1997).
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3. A. Martinez, H. C. Mireles, and I. I. Smalyukh, “Large-area optoelastic manipulation of colloidal particles in liquid crystals using photoresponsive molecular surface monolayers,” Proc. Natl. Acad. Sci. U.S.A.108(52), 20891–20896 (2011).
4. Y. Gu and N. L. Abbott, “Observation of saturn-ring defects around solid microspheres in nematic liquid crystals,” Phys. Rev. Lett.85(22), 4719–4722 (2000).
5. S. J. Woltman, G. D. Jay, and G. P. Crawford, “Liquid-crystal materials find a new order in biomedical applications,” Nat. Mater.6(12), 929–938 (2007).
6. C. P. Lapointe, T. G. Mason, and I. I. Smalyukh, “Shape-controlled colloidal interactions in nematic liquid crystals,” Science326(5956), 1083–1086 (2009).
7. J. S. Evans, C. Beier, and I. I. Smalyukh, “Alignment of high-aspect ratio colloidal gold nanoplatelets in nematic liquid crsytals,” J. Appl. Phys.110(3), 033535 (2011).
8. T. Yamamoto, Y. Tabe, and H. Yokoyama, “Manipulation of defect structures and colloidal chains in liquid crystals by means of photochemical reactions of azobenzene compounds,” Colloids Surf. A Physicochem. Eng. Asp.334, 155–159 (2009).
9. Q. Liu, Y. Cui, D. Gardner, X. Li, S. He, and I. I. Smalyukh, “Self-alignment of plasmonic gold nanorods in reconfigurable anisotropic fluids for tunable bulk metamaterial applications,” Nano Lett.10(4), 1347–1353 (2010).
10. G. M. Koenig, I.-H. Lin, and N. L. Abbott, “Chemoresponsive assemblies of microparticles at liquid crystalline interfaces,” Proc. Natl. Acad. Sci. U.S.A.107(9), 3998–4003 (2010).
11. M. R. Jones, R. J. Macfarlane, B. Lee, J. Zhang, K. L. Young, A. J. Senesi, and C. A. Mirkin, “DNA-nanoparticle superlattices formed from anisotropic building blocks,” Nat. Mater.9(11), 913–917 (2010).
12. P. M. Chaikin and T. C. Lubensky, Principles of Condensed Matter Physics (Cambridge University Press, 1995).
13. M. Zapotocky, L. Ramos, P. Poulin, T. C. Lubensky, and D. A. Weitz, “Particle-stabilized defect gel in cholesteric liquid crystals,” Science283(5399), 209–212 (1999).
14. M. Ravnik, G. P. Alexander, J. M. Yeomans, and S. P. Žumer, “Three-dimensional colloidal crystals in liquid crystalline blue phases,” Proc. Natl. Acad. Sci. U.S.A.108(13), 5188–5192 (2011).
15. D. Engström, R. P. Trivedi, M. Persson, K. A. Bertness, M. Goksör, and I. I. Smalyukh, “Three-dimensional imaging of liquid crystal structures and defects by means of holographic manipulation of colloidal nanowires with faceted sidewalls,” Soft Matter7(13), 6304–6312 (2011).
16. R. P. Trivedi, D. Engström, and I. I. Smalyukh, “Optical manipulation of colloids and defect structures in anisotropic liquid crystal fluids,” J. Opt.13(4), 044001 (2011).
17. B. Senyuk, J. S. Evans, P. Ackerman, T. Lee, P. Manna, L. Vigderman, E. R. Zubarev, J. van de Lagemaat, and I. I. Smalyukh, “Shape-dependent oriented trapping and scaffolding of plasmonic nanoparticles by topological defects for self-assembly of colloidal dimers in liquid crystals,” Nano Lett.12(2), 955–963 (2012).
18. A. Martinez, T. Lee, T. Asavei, H. Rubinsztein-Dunlop, and I. I. Smalyukh, “Three-dimensional complex-shaped photopolymerized microparticles at liquid crystal interfaces,” Soft Matter8(8), 2432–2437 (2012).
19. K. S. Novoselov, A. K. Geim, S. V. Morozov, D. Jiang, Y. Zhang, S. V. Dubonos, I. V. Grigorieva, and A. A. Firsov, “Electric field effect in atomically thin carbon films,” Science306(5696), 666–669 (2004).
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21. D. W. Kim, Y. H. Kim, H. S. Jeong, and H.-T. Jung, “Direct visualization of large-area graphene domains and boundaries by optical birefringency,” Nat. Nanotechnol.7, 29–34 (2012).
22. X. Wang, Y. P. Chen, and D. D. Nolte, “Strong anomalous optical dispersion of graphene: complex refractive index measured by Picometrology,” Opt. Express16(26), 22105–22112 (2008).
23. J. M. Dawlaty, S. Shivaraman, J. Strait, P. George, M. Chandrashekhar, F. Rana, M. G. Spencer, D. Veksler, and Y. Chen, “Broadband electromagnetic response and ultrafast dynamics of few-layer epitaxial graphene,” Appl. Phys. Lett.94, 172102 (2009).
24. R. P. Trivedi, I. I. Klevets, B. I. Senyuk, T. Lee, and I. I. Smalyukh, “Reconfigurable interactions and three-dimensional patterning of colloidal particles and defects in lamellar soft media,” Proc. Natl. Acad. Sci. U.S.A.109(13), 4744–4749 (2012).
25. A. I. Bishop, T. A. Nieminen, N. R. Heckenberg, and H. Rubinsztein-Dunlop, “Measurement of the total optical angular momentum transfer in optical tweezers,” Opt. Express14, 6963 (2006).
26. Y. Yang, P. D. Brimicombe, N. W. Roberts, M. R. Dickinson, M. Osipov, and H. F. Gleeson, “Continuously rotating chiral liquid crystal droplets in a linearly polarized laser trap,” Opt. Express16(10), 6877–6882 (2008).
27. P. Galajda and P. Ormos, “Complex micromachines produced and driven by light,” Appl. Phys. Lett.78(2), 249–251 (2001).
28. K. D. Bonin, B. Kourmanov, and T. G. Walker, “Light torque nanocontrol, nanomotors and nanorockers,” Opt. Express10(19), 984–989 (2002).
29. P. H. Jones, F. Palmisano, F. Bonaccorso, P. G. Gucciardi, G. Calogero, A. C. Ferrari, and O. M. Maragó, “Rotation detection in light-driven nanorotors,” ACS Nano3(10), 3077–3084 (2009).
30. S. H. Simpson, D. C. Benito, and S. Hanna, “Polarization-induced torque in optical traps,” Phys. Rev. A76(4), 043408 (2007).
31. B. Senyuk, Q. Liu, S. He, R. D. Kamien, R.B. Kusner, T. C. Lubensky, and I. I. Smalyukh. “Topological colloids.” doi:10.1038/nature11710 (2012). [CrossRef]
32. S. Stankovich, D. A. Dikin, G. H. B. Dommett, K. M. Kohlhaas, E. J. Zimney, E. A. Stach, R. D. Piner, S. T. Nguyen, and R. S. Ruoff, “Graphene-based composite materials,” Nature442(7100), 282–286 (2006).
33. P. Blake, P. D. Brimicombe, R. R. Nair, T. J. Booth, D. Jiang, F. Schedin, L. A. Ponomarenko, S. V. Morozov, H. F. Gleeson, E. W. Hill, A. K. Geim, and K. S. Novoselov, “Graphene-based liquid crystal device,” Nano Lett.8(6), 1704–1708 (2008).
34. F. Bonaccorso, Z. Sun, T. Hasan, and A. C. Ferrari, “Graphene photonics and optoelectronics,” Nat. Photonics4(9), 611–622 (2010).
35. Q. Liu, T. Asavei, T. Lee, H. Rubinsztein-Dunlop, S. He, and I. I. Smalyukh, “Measurement of viscosity of lyotropic liquid crystals by means of rotating laser-trapped microparticles,” Opt. Express19(25), 25134–25143 (2011).

ACS Nano

• O. M. Maragó, F. Bonaccorso, R. Saija, G. Privitera, P. G. Gucciardi, M. A. Iatì, G. Calogero, P. H. Jones, F. Borghese, P. Denti, V. Nicolosi, and A. C. Ferrari, “Brownian motion of graphene,” ACS Nano4(12), 7515–7523 (2010).
• P. H. Jones, F. Palmisano, F. Bonaccorso, P. G. Gucciardi, G. Calogero, A. C. Ferrari, and O. M. Maragó, “Rotation detection in light-driven nanorotors,” ACS Nano3(10), 3077–3084 (2009).

Appl. Phys. Lett.

• J. M. Dawlaty, S. Shivaraman, J. Strait, P. George, M. Chandrashekhar, F. Rana, M. G. Spencer, D. Veksler, and Y. Chen, “Broadband electromagnetic response and ultrafast dynamics of few-layer epitaxial graphene,” Appl. Phys. Lett.94, 172102 (2009).
• P. Galajda and P. Ormos, “Complex micromachines produced and driven by light,” Appl. Phys. Lett.78(2), 249–251 (2001).

Colloids Surf. A Physicochem. Eng. Asp.

• T. Yamamoto, Y. Tabe, and H. Yokoyama, “Manipulation of defect structures and colloidal chains in liquid crystals by means of photochemical reactions of azobenzene compounds,” Colloids Surf. A Physicochem. Eng. Asp.334, 155–159 (2009).

J. Appl. Phys.

• J. S. Evans, C. Beier, and I. I. Smalyukh, “Alignment of high-aspect ratio colloidal gold nanoplatelets in nematic liquid crsytals,” J. Appl. Phys.110(3), 033535 (2011).

J. Opt.

• R. P. Trivedi, D. Engström, and I. I. Smalyukh, “Optical manipulation of colloids and defect structures in anisotropic liquid crystal fluids,” J. Opt.13(4), 044001 (2011).

Nano Lett.

• B. Senyuk, J. S. Evans, P. Ackerman, T. Lee, P. Manna, L. Vigderman, E. R. Zubarev, J. van de Lagemaat, and I. I. Smalyukh, “Shape-dependent oriented trapping and scaffolding of plasmonic nanoparticles by topological defects for self-assembly of colloidal dimers in liquid crystals,” Nano Lett.12(2), 955–963 (2012).
• Q. Liu, Y. Cui, D. Gardner, X. Li, S. He, and I. I. Smalyukh, “Self-alignment of plasmonic gold nanorods in reconfigurable anisotropic fluids for tunable bulk metamaterial applications,” Nano Lett.10(4), 1347–1353 (2010).
• P. Blake, P. D. Brimicombe, R. R. Nair, T. J. Booth, D. Jiang, F. Schedin, L. A. Ponomarenko, S. V. Morozov, H. F. Gleeson, E. W. Hill, A. K. Geim, and K. S. Novoselov, “Graphene-based liquid crystal device,” Nano Lett.8(6), 1704–1708 (2008).

Nat. Mater.

• S. J. Woltman, G. D. Jay, and G. P. Crawford, “Liquid-crystal materials find a new order in biomedical applications,” Nat. Mater.6(12), 929–938 (2007).
• M. R. Jones, R. J. Macfarlane, B. Lee, J. Zhang, K. L. Young, A. J. Senesi, and C. A. Mirkin, “DNA-nanoparticle superlattices formed from anisotropic building blocks,” Nat. Mater.9(11), 913–917 (2010).

Nat. Nanotechnol.

• D. W. Kim, Y. H. Kim, H. S. Jeong, and H.-T. Jung, “Direct visualization of large-area graphene domains and boundaries by optical birefringency,” Nat. Nanotechnol.7, 29–34 (2012).

Nat. Photonics

• F. Bonaccorso, Z. Sun, T. Hasan, and A. C. Ferrari, “Graphene photonics and optoelectronics,” Nat. Photonics4(9), 611–622 (2010).

Nature

• S. Stankovich, D. A. Dikin, G. H. B. Dommett, K. M. Kohlhaas, E. J. Zimney, E. A. Stach, R. D. Piner, S. T. Nguyen, and R. S. Ruoff, “Graphene-based composite materials,” Nature442(7100), 282–286 (2006).

Opt. Express

• Q. Liu, T. Asavei, T. Lee, H. Rubinsztein-Dunlop, S. He, and I. I. Smalyukh, “Measurement of viscosity of lyotropic liquid crystals by means of rotating laser-trapped microparticles,” Opt. Express19(25), 25134–25143 (2011).
• X. Wang, Y. P. Chen, and D. D. Nolte, “Strong anomalous optical dispersion of graphene: complex refractive index measured by Picometrology,” Opt. Express16(26), 22105–22112 (2008).
• K. D. Bonin, B. Kourmanov, and T. G. Walker, “Light torque nanocontrol, nanomotors and nanorockers,” Opt. Express10(19), 984–989 (2002).
• A. I. Bishop, T. A. Nieminen, N. R. Heckenberg, and H. Rubinsztein-Dunlop, “Measurement of the total optical angular momentum transfer in optical tweezers,” Opt. Express14, 6963 (2006).
• Y. Yang, P. D. Brimicombe, N. W. Roberts, M. R. Dickinson, M. Osipov, and H. F. Gleeson, “Continuously rotating chiral liquid crystal droplets in a linearly polarized laser trap,” Opt. Express16(10), 6877–6882 (2008).

Phys. Rev. A

• S. H. Simpson, D. C. Benito, and S. Hanna, “Polarization-induced torque in optical traps,” Phys. Rev. A76(4), 043408 (2007).

Phys. Rev. E Stat. Phys. Plasmas Fluids Relat. Interdiscip. Topics

• P. Poulin and D. A. Weitz, “Inverted and multiple nematic emulsions,” Phys. Rev. E Stat. Phys. Plasmas Fluids Relat. Interdiscip. Topics57(1), 626–637 (1998).

Phys. Rev. Lett.

• Y. Gu and N. L. Abbott, “Observation of saturn-ring defects around solid microspheres in nematic liquid crystals,” Phys. Rev. Lett.85(22), 4719–4722 (2000).

Proc. Natl. Acad. Sci. U.S.A.

• A. Martinez, H. C. Mireles, and I. I. Smalyukh, “Large-area optoelastic manipulation of colloidal particles in liquid crystals using photoresponsive molecular surface monolayers,” Proc. Natl. Acad. Sci. U.S.A.108(52), 20891–20896 (2011).
• G. M. Koenig, I.-H. Lin, and N. L. Abbott, “Chemoresponsive assemblies of microparticles at liquid crystalline interfaces,” Proc. Natl. Acad. Sci. U.S.A.107(9), 3998–4003 (2010).
• M. Ravnik, G. P. Alexander, J. M. Yeomans, and S. P. Žumer, “Three-dimensional colloidal crystals in liquid crystalline blue phases,” Proc. Natl. Acad. Sci. U.S.A.108(13), 5188–5192 (2011).
• R. P. Trivedi, I. I. Klevets, B. I. Senyuk, T. Lee, and I. I. Smalyukh, “Reconfigurable interactions and three-dimensional patterning of colloidal particles and defects in lamellar soft media,” Proc. Natl. Acad. Sci. U.S.A.109(13), 4744–4749 (2012).

Science

• K. S. Novoselov, A. K. Geim, S. V. Morozov, D. Jiang, Y. Zhang, S. V. Dubonos, I. V. Grigorieva, and A. A. Firsov, “Electric field effect in atomically thin carbon films,” Science306(5696), 666–669 (2004).
• M. Zapotocky, L. Ramos, P. Poulin, T. C. Lubensky, and D. A. Weitz, “Particle-stabilized defect gel in cholesteric liquid crystals,” Science283(5399), 209–212 (1999).
• C. P. Lapointe, T. G. Mason, and I. I. Smalyukh, “Shape-controlled colloidal interactions in nematic liquid crystals,” Science326(5956), 1083–1086 (2009).
• P. Poulin, H. Stark, T. C. Lubensky, and D. A. Weitz, “Novel colloidal interactions in anisotropic fluids,” Science275(5307), 1770–1773 (1997).

Soft Matter

• D. Engström, R. P. Trivedi, M. Persson, K. A. Bertness, M. Goksör, and I. I. Smalyukh, “Three-dimensional imaging of liquid crystal structures and defects by means of holographic manipulation of colloidal nanowires with faceted sidewalls,” Soft Matter7(13), 6304–6312 (2011).
• A. Martinez, T. Lee, T. Asavei, H. Rubinsztein-Dunlop, and I. I. Smalyukh, “Three-dimensional complex-shaped photopolymerized microparticles at liquid crystal interfaces,” Soft Matter8(8), 2432–2437 (2012).

Other

• P. M. Chaikin and T. C. Lubensky, Principles of Condensed Matter Physics (Cambridge University Press, 1995).
• B. Senyuk, Q. Liu, S. He, R. D. Kamien, R.B. Kusner, T. C. Lubensky, and I. I. Smalyukh. “Topological colloids.” doi:10.1038/nature11710 (2012). [CrossRef]

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