Abstract

We report on observation of high-order optical nonlinearities in our recently developed photopolymerizable semiconductor CdSe quantum dot (QD)-polymer nanocomposite films at various volume fractions of CdSe QDs as high as 0.91 vol.% (3.6 wt.%). We performed Z-scan and degenerate multi-wave mixing (DMWM) measurements using a 532-nm picosecond laser delivering single 35 ps pulses at a repetition rate of 10 Hz. Using the uniformly cured polymer nanocomposite films, we observed the third- and fifth-order nonlinear optical effects in closed-aperture Z-scan measurements by which it was found that saturable nonlinear absorption (light-induced transparency) and large negative nonlinear refraction were induced. We also measured dependences of the effective third- and fifth-order nonlinear refraction constants on CdSe QD volume fraction. Based on the Maxwell-Garnett model, we estimated the third- and fifth-order nonlinear optical susceptibilities of CdSe QD and discussed a contribution of the third-order effect to the fifth-order one due to the cascaded (local-field) effect. Coexistence of the third- and fifth-order nonlinear refraction was also confirmed by DMWM.

© 2012 OSA

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2011

J. Klepp, C. Pruner, Y. Tomita, C. Plonka-Spehr, P. Geltenbort, S. Ivanov, G. Manzin, K. H. Andersen, J. Kohlbrecher, M. A. Ellabban, and M. Fally, “Diffraction of slow neutrons by holographic SiO2 nanoparticlepolymer composite gratings,” Phys. Rev. A84(1), 013621 (2011).
[CrossRef]

E. Hata, K. Mitsube, K. Momose, and Y. Tomita, “Holographic nanoparticle-polymer composites based on step-growth thiol-ene photopolymerization,” Opt. Mater. Express1(2), 207–222 (2011), http://www.opticsinfobase.org/ome/abstract.cfm?uri=ome-1-2-207 .
[CrossRef]

2010

I. Dancus, V. I. Vlad, A. Petris, N. Gaponik, V. Lesnyak, and A. Eychmüller, “Saturated near-resonant refractive optical nonlinearity in CdTe quantum dots,” Opt. Lett.35(7), 1079–1081 (2010).
[CrossRef] [PubMed]

X. Liu, K. Matsumura, Y. Tomita, K. Yasui, K. Kojima, and K. Chikama, “Nonlinear optical responses of nanoparticle-polymer composites incorporating organic (hyperbranched polymer)-metallic nanoparticle complex,” J. Appl. Phys.108(7), 073102 (2010).
[CrossRef]

M. Fally, J. Klepp, Y. Tomita, T. Nakamura, C. Pruner, M. A. Ellabban, R. A. Rupp, M. Bichler, I. D. Olenik, J. Kohlbrecher, H. Eckerlebe, H. Lemmel, and H. Rauch, “Neutron optical beam splitter from holographically structured nanoparticle-polymer composites,” Phys. Rev. Lett.105(12), 123904 (2010).
[CrossRef] [PubMed]

2009

X. Liu, Y. Tomita, J. Oshima, K. Chikama, K. Matsubara, T. Nakashima, and T. Kawai, “Holographic assembly of semiconductor CdSe quantum dots in polymer for volume Bragg grating structures with diffraction efficiency near 100%,” Appl. Phys. Lett.95(26), 261109 (2009).
[CrossRef]

K. Dolgaleva, H. Shin, and R. W. Boyd, “Observation of a microscopic cascaded contribution to the fifth-order nonlinear susceptibility,” Phys. Rev. Lett.103(11), 113902 (2009).
[CrossRef] [PubMed]

B. Gu, W. Ji, X. Q. Huang, P. S. Patil, and S. M. Dharmaprakash, “Nonlinear optical properties of 2,4,5-Trimethoxy-4-nitrochalcone: observation of two-photon-induced excited-state nonlinearities,” Opt. Express17(2), 1126–1135 (2009).
[CrossRef] [PubMed]

2008

2007

V. S. Dneprovskii, E. A. Zhukov, D. A. Kabanin, V. L. Lyaskovskii, A. V. Rakova, and T. Wumaier, “Nonlinear absorption and refraction of light in a colloidal solution of CdSe/ZnS quantum dots upon two-photon resonant excitation,” Phys. Solid State49(2), 366–370 (2007).
[CrossRef]

Z. Q. Zhang, W. Q. He, C. M. Gu, W. Z. Shen, H. Ogawa, and Q. X. Guo, “Determination of the third- and fifth-order nonlinear refractive indices in InN thin films,” Appl. Phys. Lett.91(22), 221902 (2007).
[CrossRef]

N. Venkatram, R. Sathyavathi, and D. N. Rao, “Size dependent multiphoton absorption and refraction of CdSe nanoparticles,” Opt. Express15(19), 12258–12263 (2007).
[CrossRef] [PubMed]

E. L. Falcão-Filho, B. de Araújo, J. J. Rodrigues, and Jr., “High-order nonlinearities of aqueous colloids containing silver nanoparticles,” J. Opt. Soc. Am. B24(12), 2948–2956 (2007).

L. Pan, N. Tamai, K. Kamada, and S. Deki, “Nonlinear optical properties of thiol-capped CdTe quantum dots in nonresonant region,” Appl. Phys. Lett.91(5), 051902 (2007).
[CrossRef]

2006

Z. Zhang, P. Zhao, P. Lin, and F. Sun, “Thermo-optic coefficients of polymers for optical waveguide applications,” Polymer (Guildf.)47(14), 4893–4896 (2006).
[CrossRef]

B. Gu, Y. Fan, J. Wang, J. Chen, J. Ding, H. Wang, and B. Guo, “Characterization of saturable absorbers using an open-aperture Gaussian-beam Z scan,” Phys. Rev. A73(6), 065803 (2006).
[CrossRef]

Y. Chen, K. Beckwitt, F. W. Wise, B. G. Aitken, J. S. Sanghera, and I. D. Aggarwal, “Measurement of fifth- and seventh-order nonlinearities of glasses,” J. Opt. Soc. Am. B23(2), 347–352 (2006).
[CrossRef]

N. Suzuki, Y. Tomita, K. Ohmori, M. Hidaka, and K. Chikama, “Highly transparent ZrO(2) nanoparticle-dispersed acrylate photopolymers for volume holographic recording,” Opt. Express14(26), 12712–12719 (2006), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-14-26-12712 .
[CrossRef] [PubMed]

H. S. Kim, M. H. Lee, N. C. Jeong, S. M. Lee, B. K. Rhee, and K. B. Yoon, “Very high third-order nonlinear optical activities of intrazeolite PbS quantum dots,” J. Am. Chem. Soc.128(47), 15070–15071 (2006).
[CrossRef] [PubMed]

J. Seo, S. Ma, Q. Yang, L. Creekmore, R. Battle, H. Brown, A. Jackson, T. Skyles, B. Tabibi, W. Yu, S. Jung, and M. Namkung, “Large resonant third-order optical nonlinearity of CdSe nanocrystal quantum dots,” J. Phys.: Conf. Ser.38, 91–94 (2006).
[CrossRef]

S. M. Ma, J. T. Seo, Q. Yang, R. Battle, H. Brown, K. Lee, L. Creekmore, A. Jackson, T. Skyles, B. Tabibi, S. S. Jung, W. Yu, and M. Namkung, “Third-order nonlinear susceptibility and hyperpolarizability of CdSe nanocrystals with femtosecond excitation,” J. Korean Phys. Soc.48(6), 1379–1384 (2006).

2005

I. Gerdova and A. Haché, “Third-order non-linear spectroscopy of CdSe and CdSe/ZnS core shell quantum dots,” Opt. Commun.246(1–3), 205–212 (2005).
[CrossRef]

Y. Tomita, “Holographic manipulation of nanoparticle-distribution morphology in photopolymers and its applications to volume holographic recording and nonlinear photonic crystals,” OSA Trends Opt. Photonics Ser.99, 274–280 (2005).

T. Nakashima, T. Sakakibara, and T. Kawai, “Highly luminescent CdTe nanocrystal-polymer composites based on ionic liquid,” Chem. Lett.34(10), 1410–1411 (2005).
[CrossRef]

J. He, J. Mi, H. Li, and W. Ji, “Observation of interband two-photon absorption saturation in CdS nanocrystals,” J. Phys. Chem. B109(41), 19184–19187 (2005).
[CrossRef] [PubMed]

N. Venkatram, D. N. Rao, and M. A. Akundi, “Nonlinear absorption, scattering and optical limiting studies of CdS nanoparticles,” Opt. Express13(3), 867–872 (2005).
[CrossRef] [PubMed]

Y. Tomita, N. Suzuki, and K. Chikama, “Holographic manipulation of nanoparticle distribution morphology in nanoparticle-dispersed photopolymers,” Opt. Lett.30(8), 839–841 (2005).
[CrossRef] [PubMed]

L. A. Padilha, J. Fu, D. J. Hagan, E. W. Van Stryland, C. L. Cesar, L. C. Barbosa, and C. H. B. Cruz, “Two-photon absorption in CdTe quantum dots,” Opt. Express13(17), 6460–6467 (2005).
[CrossRef] [PubMed]

B. Gu, J. Chen, Y. X. Fan, J. Ding, and H. T. Wang, “Theory of Gaussian beam Z scan with simultaneous third- and fifth-order nonlinear refraction based on a Gaussian decomposition method,” J. Opt. Soc. Am. B22(12), 2651–2659 (2005).
[CrossRef]

2004

Y. Lin, J. Zhang, E. Kumacheva, and E. H. Sargent, “Third-order optical nonlinearity and figure of merit of CdS nanocrystals chemically stabilized in spin-processable polymer films,” J. Mater. Sci.39(3), 993–996 (2004).
[CrossRef]

2003

2002

2001

K. S. Bindra and A. K. Kar, “Role of femtosecond pulses in distinguishing third- and fifth-order nonlinearity for semiconductor-doped glasses,” Appl. Phys. Lett.79(23), 3761–3763 (2001).
[CrossRef]

B. Liu, H. Li, C. H. Chew, W. Que, Y. L. Lam, C. H. Kam, L. M. Gan, and G. Q. Xu, “PbS–polymer nanocomposite with third-order nonlinear optical response in femtosecond regime,” Mater. Lett.51(6), 461–469 (2001).
[CrossRef]

2000

F. Smektala, C. Quemard, V. Couderc, and A. Barthélémy, “Non-linear optical properties of chalcogenide glasses measured by Z-scan,” J. Non-Cryst. Solids274(1–3), 232–237 (2000).
[CrossRef]

F. Sanchez, K. Abbaoui, and Y. Cherruault, “Beyond the thin-sheet approximation: Adomian’s decomposition,” Opt. Commun.173(1-6), 397–401 (2000).
[CrossRef]

1999

C. Burda, S. Link, T. C. Green, and M. A. El-Sayed, “New transient absorption observed in the spectrum of colloidal CdSe nanoparticles pumped with high-power femtosecond pulses,” J. Phys. Chem. B103(49), 10775–10780 (1999).
[CrossRef]

1998

G. P. Banfi, V. Degiorgio, and D. Ricard, “Nonlinear optical properties of semiconductor nanocrystals,” Adv. Phys.47(3), 447–510 (1998) (and references therein).
[CrossRef]

1997

E. Koudoumas, F. Dong, S. Couris, and S. Leach, “High order nonlinear optical response of fullerene solutions in the nanosecond regime,” Opt. Commun.138(4–6), 301–304 (1997).
[CrossRef]

1996

E. Koudoumas, F. Dong, M. D. tzatzadaki, S. Couris, and S. Leach, “High-order nonlinear optical response of C60-toluene solutions in the sub-picosecond regime,” J. Phys. At. Mol. Opt. Phys.29(20), L773–L778 (1996).
[CrossRef]

G. Lowet and G. Van der Perre, “Ultrasound velocity measurement in long bones: measurement method and simulation of ultrasound wave propagation,” J. Biomech.29(10), 1255–1262 (1996).
[CrossRef] [PubMed]

B. Taheri, H. Liu, B. Jassemnejad, D. Appling, R. C. Powell, and J. J. Song, “Intensity scan and two photon absorption and nonlinear refraction of C60 in toluene,” Appl. Phys. Lett.68(10), 1317–1319 (1996).
[CrossRef]

L. W. Wang and A. Zunger, “Pseudopotential calculations of nanoscale CdSe quantum dots,” Phys. Rev. B Condens. Matter53(15), 9579–9582 (1996).
[CrossRef] [PubMed]

1995

M. D. Dvorak, B. L. Justus, and A. D. Berry, “Pump/probe Z-scan studies of GaAs nanocrystals grown in porous glass,” Opt. Commun.116(1–3), 149–152 (1995).
[CrossRef]

W. Schmid, T. Vogtmann, and M. Schwoere, “A modulation technique for measuring the optical susceptibility χ(5) by degenerate four-wave mixing,” Opt. Commun.121(1–3), 55–62 (1995).
[CrossRef]

G. P. Banfi, V. Degiorgio, and H. M. Tan, “Optical nonlinearity of semiconductor-doped glasses at frequencies below the band gap: the role of free carriers,” J. Opt. Soc. Am. B12(4), 621–628 (1995).
[CrossRef]

1993

S. H. Park, M. P. Casey, and J. Falk, “Nonlinear optical properties of CdSe quantum dots,” J. Appl. Phys.73(12), 8041–8045 (1993).
[CrossRef]

1991

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of Bound Electronic Nonlinear Refraction in Solids,” IEEE J. Quantum Electron.27(6), 1296–1309 (1991).
[CrossRef]

1990

S. H. Park, R. A. Morgan, Y. Z. Hu, M. Lindberg, S. W. Koch, and N. Peyghambarian, “Nonlinear optical properties of quantum-confined CdSe microcrystallites,” J. Opt. Soc. Am. B7(10), 2097–2105 (1990).
[CrossRef]

J. Yumoto, H. Shinojima, N. Uesugi, K. Tsunetomo, H. Nasu, and Y. Osaka, “Optical nonlinearity of CdSe microcrystallites in a sputtered SiO2 film,” Appl. Phys. Lett.57(23), 2393–2395 (1990).
[CrossRef]

L. H. Acioli, A. S. L. Gomes, J. R. Rios Leite, and C. B. De Araujo, “ultrafast χ(3)-related processes in semiconductor doped glasses,” IEEE J. Quantum Electron.26(7), 1277–1284 (1990).
[CrossRef]

M. G. Bawendi, W. L. Wilson, L. Rothberg, P. J. Carroll, T. M. Jedju, M. L. Steigerwald, and L. E. Brus, “Electronic structure and photoexcited-carrier dynamics in nanometer-size CdSe clusters,” Phys. Rev. Lett.65(13), 1623–1626 (1990).
[CrossRef] [PubMed]

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive Measurement of Optical Nonlinearities Using a Single Beam,” IEEE J. Quantum Electron.26(4), 760–769 (1990).
[CrossRef]

1989

N. Peyghambarian, B. Fluegel, D. Hulin, A. Migus, M. Joffre, A. Antonetti, S. W. Koch, and M. Lindberg, “Femtosecond optical nonlinearities of CdSe quantum dots,” IEEE J. Quantum Electron.25(12), 2516–2522 (1989).
[CrossRef]

G. I. Stegeman and R. H. Stolen, “Waveguides and fibers for nonlinear optics,” J. Opt. Soc. Am. B6(4), 652–662 (1989).
[CrossRef]

1988

G. Adomian, “A review of the decomposition method in applied mathematics,” J. Math. Anal. Appl.135(2), 501–544 (1988).
[CrossRef]

Y. Kayanuma, “Quantum-size effects of interacting electrons and holes in semiconductor microcrystals with spherical shape,” Phys. Rev. B Condens. Matter38(14), 9797–9805 (1988).
[CrossRef] [PubMed]

L. H. Acioli, A. S. L. Gomes, and J. R. Rios Leite, “Measurement of high-order optical nonlinear susceptibilities in semiconductor-doped glasses,” Appl. Phys. Lett.53(19), 1788–1790 (1988).
[CrossRef]

1987

S. Schumitt-Rink, D. A. B. Miller, and D. S. Chemla, “Theory of the linear and nonlinear optical properties of semiconductor microcrystallites,” Phys. Rev. B35(15), 8113–8125 (1987).
[CrossRef]

S. R. Friberg and P. W. Smith, “Nonlinear optical glasses for ultrafast optical switches,” IEEE J. Quantum Electron.23(12), 2089–2094 (1987).
[CrossRef]

1978

Abbaoui, K.

F. Sanchez, K. Abbaoui, and Y. Cherruault, “Beyond the thin-sheet approximation: Adomian’s decomposition,” Opt. Commun.173(1-6), 397–401 (2000).
[CrossRef]

Acioli, L. H.

L. H. Acioli, A. S. L. Gomes, J. R. Rios Leite, and C. B. De Araujo, “ultrafast χ(3)-related processes in semiconductor doped glasses,” IEEE J. Quantum Electron.26(7), 1277–1284 (1990).
[CrossRef]

L. H. Acioli, A. S. L. Gomes, and J. R. Rios Leite, “Measurement of high-order optical nonlinear susceptibilities in semiconductor-doped glasses,” Appl. Phys. Lett.53(19), 1788–1790 (1988).
[CrossRef]

Adomian, G.

G. Adomian, “A review of the decomposition method in applied mathematics,” J. Math. Anal. Appl.135(2), 501–544 (1988).
[CrossRef]

Aggarwal, I. D.

Aitken, B. G.

Akundi, M. A.

Andersen, K. H.

J. Klepp, C. Pruner, Y. Tomita, C. Plonka-Spehr, P. Geltenbort, S. Ivanov, G. Manzin, K. H. Andersen, J. Kohlbrecher, M. A. Ellabban, and M. Fally, “Diffraction of slow neutrons by holographic SiO2 nanoparticlepolymer composite gratings,” Phys. Rev. A84(1), 013621 (2011).
[CrossRef]

Antonetti, A.

N. Peyghambarian, B. Fluegel, D. Hulin, A. Migus, M. Joffre, A. Antonetti, S. W. Koch, and M. Lindberg, “Femtosecond optical nonlinearities of CdSe quantum dots,” IEEE J. Quantum Electron.25(12), 2516–2522 (1989).
[CrossRef]

Appling, D.

B. Taheri, H. Liu, B. Jassemnejad, D. Appling, R. C. Powell, and J. J. Song, “Intensity scan and two photon absorption and nonlinear refraction of C60 in toluene,” Appl. Phys. Lett.68(10), 1317–1319 (1996).
[CrossRef]

Banfi, G. P.

G. P. Banfi, V. Degiorgio, and D. Ricard, “Nonlinear optical properties of semiconductor nanocrystals,” Adv. Phys.47(3), 447–510 (1998) (and references therein).
[CrossRef]

G. P. Banfi, V. Degiorgio, and H. M. Tan, “Optical nonlinearity of semiconductor-doped glasses at frequencies below the band gap: the role of free carriers,” J. Opt. Soc. Am. B12(4), 621–628 (1995).
[CrossRef]

Barbosa, L. C.

Barthélémy, A.

F. Smektala, C. Quemard, V. Couderc, and A. Barthélémy, “Non-linear optical properties of chalcogenide glasses measured by Z-scan,” J. Non-Cryst. Solids274(1–3), 232–237 (2000).
[CrossRef]

Battle, R.

S. M. Ma, J. T. Seo, Q. Yang, R. Battle, H. Brown, K. Lee, L. Creekmore, A. Jackson, T. Skyles, B. Tabibi, S. S. Jung, W. Yu, and M. Namkung, “Third-order nonlinear susceptibility and hyperpolarizability of CdSe nanocrystals with femtosecond excitation,” J. Korean Phys. Soc.48(6), 1379–1384 (2006).

J. Seo, S. Ma, Q. Yang, L. Creekmore, R. Battle, H. Brown, A. Jackson, T. Skyles, B. Tabibi, W. Yu, S. Jung, and M. Namkung, “Large resonant third-order optical nonlinearity of CdSe nanocrystal quantum dots,” J. Phys.: Conf. Ser.38, 91–94 (2006).
[CrossRef]

Bawendi, M. G.

M. G. Bawendi, W. L. Wilson, L. Rothberg, P. J. Carroll, T. M. Jedju, M. L. Steigerwald, and L. E. Brus, “Electronic structure and photoexcited-carrier dynamics in nanometer-size CdSe clusters,” Phys. Rev. Lett.65(13), 1623–1626 (1990).
[CrossRef] [PubMed]

Beckwitt, K.

Berry, A. D.

M. D. Dvorak, B. L. Justus, and A. D. Berry, “Pump/probe Z-scan studies of GaAs nanocrystals grown in porous glass,” Opt. Commun.116(1–3), 149–152 (1995).
[CrossRef]

Bichler, M.

M. Fally, J. Klepp, Y. Tomita, T. Nakamura, C. Pruner, M. A. Ellabban, R. A. Rupp, M. Bichler, I. D. Olenik, J. Kohlbrecher, H. Eckerlebe, H. Lemmel, and H. Rauch, “Neutron optical beam splitter from holographically structured nanoparticle-polymer composites,” Phys. Rev. Lett.105(12), 123904 (2010).
[CrossRef] [PubMed]

Bindra, K. S.

K. S. Bindra and A. K. Kar, “Role of femtosecond pulses in distinguishing third- and fifth-order nonlinearity for semiconductor-doped glasses,” Appl. Phys. Lett.79(23), 3761–3763 (2001).
[CrossRef]

Boyd, R. W.

Brown, H.

S. M. Ma, J. T. Seo, Q. Yang, R. Battle, H. Brown, K. Lee, L. Creekmore, A. Jackson, T. Skyles, B. Tabibi, S. S. Jung, W. Yu, and M. Namkung, “Third-order nonlinear susceptibility and hyperpolarizability of CdSe nanocrystals with femtosecond excitation,” J. Korean Phys. Soc.48(6), 1379–1384 (2006).

J. Seo, S. Ma, Q. Yang, L. Creekmore, R. Battle, H. Brown, A. Jackson, T. Skyles, B. Tabibi, W. Yu, S. Jung, and M. Namkung, “Large resonant third-order optical nonlinearity of CdSe nanocrystal quantum dots,” J. Phys.: Conf. Ser.38, 91–94 (2006).
[CrossRef]

Brozozowski, L.

Brus, L. E.

M. G. Bawendi, W. L. Wilson, L. Rothberg, P. J. Carroll, T. M. Jedju, M. L. Steigerwald, and L. E. Brus, “Electronic structure and photoexcited-carrier dynamics in nanometer-size CdSe clusters,” Phys. Rev. Lett.65(13), 1623–1626 (1990).
[CrossRef] [PubMed]

Burda, C.

C. Burda, S. Link, T. C. Green, and M. A. El-Sayed, “New transient absorption observed in the spectrum of colloidal CdSe nanoparticles pumped with high-power femtosecond pulses,” J. Phys. Chem. B103(49), 10775–10780 (1999).
[CrossRef]

Carroll, P. J.

M. G. Bawendi, W. L. Wilson, L. Rothberg, P. J. Carroll, T. M. Jedju, M. L. Steigerwald, and L. E. Brus, “Electronic structure and photoexcited-carrier dynamics in nanometer-size CdSe clusters,” Phys. Rev. Lett.65(13), 1623–1626 (1990).
[CrossRef] [PubMed]

Casey, M. P.

S. H. Park, M. P. Casey, and J. Falk, “Nonlinear optical properties of CdSe quantum dots,” J. Appl. Phys.73(12), 8041–8045 (1993).
[CrossRef]

Cesar, C. L.

Chemla, D. S.

S. Schumitt-Rink, D. A. B. Miller, and D. S. Chemla, “Theory of the linear and nonlinear optical properties of semiconductor microcrystallites,” Phys. Rev. B35(15), 8113–8125 (1987).
[CrossRef]

Chen, J.

B. Gu, Y. Fan, J. Wang, J. Chen, J. Ding, H. Wang, and B. Guo, “Characterization of saturable absorbers using an open-aperture Gaussian-beam Z scan,” Phys. Rev. A73(6), 065803 (2006).
[CrossRef]

B. Gu, J. Chen, Y. X. Fan, J. Ding, and H. T. Wang, “Theory of Gaussian beam Z scan with simultaneous third- and fifth-order nonlinear refraction based on a Gaussian decomposition method,” J. Opt. Soc. Am. B22(12), 2651–2659 (2005).
[CrossRef]

Chen, Y.

Cherruault, Y.

F. Sanchez, K. Abbaoui, and Y. Cherruault, “Beyond the thin-sheet approximation: Adomian’s decomposition,” Opt. Commun.173(1-6), 397–401 (2000).
[CrossRef]

Chew, C. H.

B. Liu, H. Li, C. H. Chew, W. Que, Y. L. Lam, C. H. Kam, L. M. Gan, and G. Q. Xu, “PbS–polymer nanocomposite with third-order nonlinear optical response in femtosecond regime,” Mater. Lett.51(6), 461–469 (2001).
[CrossRef]

Chikama, K.

X. Liu, K. Matsumura, Y. Tomita, K. Yasui, K. Kojima, and K. Chikama, “Nonlinear optical responses of nanoparticle-polymer composites incorporating organic (hyperbranched polymer)-metallic nanoparticle complex,” J. Appl. Phys.108(7), 073102 (2010).
[CrossRef]

X. Liu, Y. Tomita, J. Oshima, K. Chikama, K. Matsubara, T. Nakashima, and T. Kawai, “Holographic assembly of semiconductor CdSe quantum dots in polymer for volume Bragg grating structures with diffraction efficiency near 100%,” Appl. Phys. Lett.95(26), 261109 (2009).
[CrossRef]

N. Suzuki, Y. Tomita, K. Ohmori, M. Hidaka, and K. Chikama, “Highly transparent ZrO(2) nanoparticle-dispersed acrylate photopolymers for volume holographic recording,” Opt. Express14(26), 12712–12719 (2006), http://www.opticsinfobase.org/oe/abstract.cfm?URI=oe-14-26-12712 .
[CrossRef] [PubMed]

Y. Tomita, N. Suzuki, and K. Chikama, “Holographic manipulation of nanoparticle distribution morphology in nanoparticle-dispersed photopolymers,” Opt. Lett.30(8), 839–841 (2005).
[CrossRef] [PubMed]

Couderc, V.

F. Smektala, C. Quemard, V. Couderc, and A. Barthélémy, “Non-linear optical properties of chalcogenide glasses measured by Z-scan,” J. Non-Cryst. Solids274(1–3), 232–237 (2000).
[CrossRef]

Couris, S.

E. Koudoumas, F. Dong, S. Couris, and S. Leach, “High order nonlinear optical response of fullerene solutions in the nanosecond regime,” Opt. Commun.138(4–6), 301–304 (1997).
[CrossRef]

E. Koudoumas, F. Dong, M. D. tzatzadaki, S. Couris, and S. Leach, “High-order nonlinear optical response of C60-toluene solutions in the sub-picosecond regime,” J. Phys. At. Mol. Opt. Phys.29(20), L773–L778 (1996).
[CrossRef]

Creekmore, L.

S. M. Ma, J. T. Seo, Q. Yang, R. Battle, H. Brown, K. Lee, L. Creekmore, A. Jackson, T. Skyles, B. Tabibi, S. S. Jung, W. Yu, and M. Namkung, “Third-order nonlinear susceptibility and hyperpolarizability of CdSe nanocrystals with femtosecond excitation,” J. Korean Phys. Soc.48(6), 1379–1384 (2006).

J. Seo, S. Ma, Q. Yang, L. Creekmore, R. Battle, H. Brown, A. Jackson, T. Skyles, B. Tabibi, W. Yu, S. Jung, and M. Namkung, “Large resonant third-order optical nonlinearity of CdSe nanocrystal quantum dots,” J. Phys.: Conf. Ser.38, 91–94 (2006).
[CrossRef]

Cruz, C. H. B.

Dancus, I.

De Araujo, C. B.

L. H. Acioli, A. S. L. Gomes, J. R. Rios Leite, and C. B. De Araujo, “ultrafast χ(3)-related processes in semiconductor doped glasses,” IEEE J. Quantum Electron.26(7), 1277–1284 (1990).
[CrossRef]

de Araujo, R. E.

de Araújo, B.

Degiorgio, V.

G. P. Banfi, V. Degiorgio, and D. Ricard, “Nonlinear optical properties of semiconductor nanocrystals,” Adv. Phys.47(3), 447–510 (1998) (and references therein).
[CrossRef]

G. P. Banfi, V. Degiorgio, and H. M. Tan, “Optical nonlinearity of semiconductor-doped glasses at frequencies below the band gap: the role of free carriers,” J. Opt. Soc. Am. B12(4), 621–628 (1995).
[CrossRef]

Deki, S.

L. Pan, N. Tamai, K. Kamada, and S. Deki, “Nonlinear optical properties of thiol-capped CdTe quantum dots in nonresonant region,” Appl. Phys. Lett.91(5), 051902 (2007).
[CrossRef]

Dharmaprakash, S. M.

Ding, J.

B. Gu, Y. Fan, J. Wang, J. Chen, J. Ding, H. Wang, and B. Guo, “Characterization of saturable absorbers using an open-aperture Gaussian-beam Z scan,” Phys. Rev. A73(6), 065803 (2006).
[CrossRef]

B. Gu, J. Chen, Y. X. Fan, J. Ding, and H. T. Wang, “Theory of Gaussian beam Z scan with simultaneous third- and fifth-order nonlinear refraction based on a Gaussian decomposition method,” J. Opt. Soc. Am. B22(12), 2651–2659 (2005).
[CrossRef]

Dneprovskii, V. S.

V. S. Dneprovskii, E. A. Zhukov, D. A. Kabanin, V. L. Lyaskovskii, A. V. Rakova, and T. Wumaier, “Nonlinear absorption and refraction of light in a colloidal solution of CdSe/ZnS quantum dots upon two-photon resonant excitation,” Phys. Solid State49(2), 366–370 (2007).
[CrossRef]

Dolgaleva, K.

K. Dolgaleva, H. Shin, and R. W. Boyd, “Observation of a microscopic cascaded contribution to the fifth-order nonlinear susceptibility,” Phys. Rev. Lett.103(11), 113902 (2009).
[CrossRef] [PubMed]

Dong, F.

E. Koudoumas, F. Dong, S. Couris, and S. Leach, “High order nonlinear optical response of fullerene solutions in the nanosecond regime,” Opt. Commun.138(4–6), 301–304 (1997).
[CrossRef]

E. Koudoumas, F. Dong, M. D. tzatzadaki, S. Couris, and S. Leach, “High-order nonlinear optical response of C60-toluene solutions in the sub-picosecond regime,” J. Phys. At. Mol. Opt. Phys.29(20), L773–L778 (1996).
[CrossRef]

Dvorak, M. D.

M. D. Dvorak, B. L. Justus, and A. D. Berry, “Pump/probe Z-scan studies of GaAs nanocrystals grown in porous glass,” Opt. Commun.116(1–3), 149–152 (1995).
[CrossRef]

Eckerlebe, H.

M. Fally, J. Klepp, Y. Tomita, T. Nakamura, C. Pruner, M. A. Ellabban, R. A. Rupp, M. Bichler, I. D. Olenik, J. Kohlbrecher, H. Eckerlebe, H. Lemmel, and H. Rauch, “Neutron optical beam splitter from holographically structured nanoparticle-polymer composites,” Phys. Rev. Lett.105(12), 123904 (2010).
[CrossRef] [PubMed]

Ellabban, M. A.

J. Klepp, C. Pruner, Y. Tomita, C. Plonka-Spehr, P. Geltenbort, S. Ivanov, G. Manzin, K. H. Andersen, J. Kohlbrecher, M. A. Ellabban, and M. Fally, “Diffraction of slow neutrons by holographic SiO2 nanoparticlepolymer composite gratings,” Phys. Rev. A84(1), 013621 (2011).
[CrossRef]

M. Fally, J. Klepp, Y. Tomita, T. Nakamura, C. Pruner, M. A. Ellabban, R. A. Rupp, M. Bichler, I. D. Olenik, J. Kohlbrecher, H. Eckerlebe, H. Lemmel, and H. Rauch, “Neutron optical beam splitter from holographically structured nanoparticle-polymer composites,” Phys. Rev. Lett.105(12), 123904 (2010).
[CrossRef] [PubMed]

El-Sayed, M. A.

C. Burda, S. Link, T. C. Green, and M. A. El-Sayed, “New transient absorption observed in the spectrum of colloidal CdSe nanoparticles pumped with high-power femtosecond pulses,” J. Phys. Chem. B103(49), 10775–10780 (1999).
[CrossRef]

Eychmüller, A.

Falcão-Filho, E. L.

Falk, J.

S. H. Park, M. P. Casey, and J. Falk, “Nonlinear optical properties of CdSe quantum dots,” J. Appl. Phys.73(12), 8041–8045 (1993).
[CrossRef]

Fally, M.

J. Klepp, C. Pruner, Y. Tomita, C. Plonka-Spehr, P. Geltenbort, S. Ivanov, G. Manzin, K. H. Andersen, J. Kohlbrecher, M. A. Ellabban, and M. Fally, “Diffraction of slow neutrons by holographic SiO2 nanoparticlepolymer composite gratings,” Phys. Rev. A84(1), 013621 (2011).
[CrossRef]

M. Fally, J. Klepp, Y. Tomita, T. Nakamura, C. Pruner, M. A. Ellabban, R. A. Rupp, M. Bichler, I. D. Olenik, J. Kohlbrecher, H. Eckerlebe, H. Lemmel, and H. Rauch, “Neutron optical beam splitter from holographically structured nanoparticle-polymer composites,” Phys. Rev. Lett.105(12), 123904 (2010).
[CrossRef] [PubMed]

Fan, Y.

B. Gu, Y. Fan, J. Wang, J. Chen, J. Ding, H. Wang, and B. Guo, “Characterization of saturable absorbers using an open-aperture Gaussian-beam Z scan,” Phys. Rev. A73(6), 065803 (2006).
[CrossRef]

Fan, Y. X.

Fluegel, B.

N. Peyghambarian, B. Fluegel, D. Hulin, A. Migus, M. Joffre, A. Antonetti, S. W. Koch, and M. Lindberg, “Femtosecond optical nonlinearities of CdSe quantum dots,” IEEE J. Quantum Electron.25(12), 2516–2522 (1989).
[CrossRef]

Friberg, S. R.

S. R. Friberg and P. W. Smith, “Nonlinear optical glasses for ultrafast optical switches,” IEEE J. Quantum Electron.23(12), 2089–2094 (1987).
[CrossRef]

Fu, J.

Gan, C.

C. Gan, Y. Zhang, S. W. Liu, Y. Wang, and M. Xiao, “Linear and nonlinear optical refractions of CR39 composite with CdSe nanocrystals,” Opt. Mater.30(9), 1440–1445 (2008).
[CrossRef]

Gan, L. M.

B. Liu, H. Li, C. H. Chew, W. Que, Y. L. Lam, C. H. Kam, L. M. Gan, and G. Q. Xu, “PbS–polymer nanocomposite with third-order nonlinear optical response in femtosecond regime,” Mater. Lett.51(6), 461–469 (2001).
[CrossRef]

Gaponik, N.

Gaylord, T. K.

Geltenbort, P.

J. Klepp, C. Pruner, Y. Tomita, C. Plonka-Spehr, P. Geltenbort, S. Ivanov, G. Manzin, K. H. Andersen, J. Kohlbrecher, M. A. Ellabban, and M. Fally, “Diffraction of slow neutrons by holographic SiO2 nanoparticlepolymer composite gratings,” Phys. Rev. A84(1), 013621 (2011).
[CrossRef]

Gerdova, I.

I. Gerdova and A. Haché, “Third-order non-linear spectroscopy of CdSe and CdSe/ZnS core shell quantum dots,” Opt. Commun.246(1–3), 205–212 (2005).
[CrossRef]

Gomes, A. S. L.

D. Rativa, R. E. de Araujo, and A. S. L. Gomes, “Nonresonant high-order nonlinear optical properties of silver nanoparticles in aqueous solution,” Opt. Express16(23), 19244–19252 (2008).
[CrossRef] [PubMed]

L. H. Acioli, A. S. L. Gomes, J. R. Rios Leite, and C. B. De Araujo, “ultrafast χ(3)-related processes in semiconductor doped glasses,” IEEE J. Quantum Electron.26(7), 1277–1284 (1990).
[CrossRef]

L. H. Acioli, A. S. L. Gomes, and J. R. Rios Leite, “Measurement of high-order optical nonlinear susceptibilities in semiconductor-doped glasses,” Appl. Phys. Lett.53(19), 1788–1790 (1988).
[CrossRef]

Green, T. C.

C. Burda, S. Link, T. C. Green, and M. A. El-Sayed, “New transient absorption observed in the spectrum of colloidal CdSe nanoparticles pumped with high-power femtosecond pulses,” J. Phys. Chem. B103(49), 10775–10780 (1999).
[CrossRef]

Gu, B.

Gu, C. M.

Z. Q. Zhang, W. Q. He, C. M. Gu, W. Z. Shen, H. Ogawa, and Q. X. Guo, “Determination of the third- and fifth-order nonlinear refractive indices in InN thin films,” Appl. Phys. Lett.91(22), 221902 (2007).
[CrossRef]

Guo, B.

B. Gu, Y. Fan, J. Wang, J. Chen, J. Ding, H. Wang, and B. Guo, “Characterization of saturable absorbers using an open-aperture Gaussian-beam Z scan,” Phys. Rev. A73(6), 065803 (2006).
[CrossRef]

Guo, Q. X.

Z. Q. Zhang, W. Q. He, C. M. Gu, W. Z. Shen, H. Ogawa, and Q. X. Guo, “Determination of the third- and fifth-order nonlinear refractive indices in InN thin films,” Appl. Phys. Lett.91(22), 221902 (2007).
[CrossRef]

Haché, A.

I. Gerdova and A. Haché, “Third-order non-linear spectroscopy of CdSe and CdSe/ZnS core shell quantum dots,” Opt. Commun.246(1–3), 205–212 (2005).
[CrossRef]

Hagan, D. J.

L. A. Padilha, J. Fu, D. J. Hagan, E. W. Van Stryland, C. L. Cesar, L. C. Barbosa, and C. H. B. Cruz, “Two-photon absorption in CdTe quantum dots,” Opt. Express13(17), 6460–6467 (2005).
[CrossRef] [PubMed]

M. Sheik-Bahae, D. C. Hutchings, D. J. Hagan, and E. W. Van Stryland, “Dispersion of Bound Electronic Nonlinear Refraction in Solids,” IEEE J. Quantum Electron.27(6), 1296–1309 (1991).
[CrossRef]

M. Sheik-Bahae, A. A. Said, T. Wei, D. J. Hagan, and E. W. Van Stryland, “Sensitive Measurement of Optical Nonlinearities Using a Single Beam,” IEEE J. Quantum Electron.26(4), 760–769 (1990).
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Figures (8)

Fig. 1
Fig. 1

Spectral linear absorption coefficients for cured polymer nanocomposite film samples at different volume fractions of CdSe QDs.

Fig. 2
Fig. 2

Experimental setup for forward DMWM. BS, a beam splitter; L, a convex lens; S, a polymer nanocomposite film sample; P, a prism. k3, k5, k3 and k5 indicate wavevetors of self-diffracted beams.

Fig. 3
Fig. 3

(a) Open-aperture Z-scan T(z) at I0 = 1.8 GW/cm2 as a function of sample position z for a polymer nanocomposite film sample with 0.91 vol.% CdSe QDs. The solid curves are the least-squares fits of the TPA (curve in red), SA1 (curve in blue) and SA2 (curve in brown) models to the data. Best fit values for the TPA, SA1 and SA2 models are β = 107 cm/GW, Is = 0.53 and 0.11 GW/cm2, respectively. (b) Transmittance change ΔT at z = 0 as a function of input intensity I0. The solid curves are the least-squares fits of the TPA (curve in red), SA1 (curve in blue) and SA2 (curve in brown) models to the data.

Fig. 4
Fig. 4

(a) Closed-aperture Z-scan T(z) at I0 = 1.8 GW/cm2 as a function of sample position z for the same polymer nanocomposite film sample with 0.91 vol.% CdSe QDs as that shown in Fig. 3. Solid curves correspond to the least-squares fits of the theoretical formulae for the closed-aperture Gaussian-beam Z-scan T(z) without (curve in red) and with (curve in blue) saturable absorption of the SA1 type. The best-fit values for n2 and n4 are −4.0 × 10−3 cm2/GW and + 1.5 × 10−3 cm4/GW2, respectively. (b) ΔTp-v/I0 as a function of input intensity I0. The solid line is the least-squares linear fit to the data.

Fig. 5
Fig. 5

(a) Extracted values for (a) n2 and (b) n4 as a function of input intensity I0 for a polymer nanocomposite film sample doped with 0.91 vol.% CdSe QDs.

Fig. 6
Fig. 6

Extracted values for (a) n2 and (b) n4 as a function of volume fraction of CdSe QDs. The solid curves are the least-squares fits to the data.

Fig. 7
Fig. 7

Closed-aperture Z-scan T(z) as a function of incident intensity for a polymer nanocomposite film sample doped with 0.91 vol.% CdSe QDs when the sample is placed at the valley (○) and peak (●) positions.

Fig. 8
Fig. 8

Far-field transmitted and diffracted beams from the polymer nanocomposite film sample with 0.91 vol.% CdSe QDs at grating spacing of (a) 40 μm and (b) 1 μm.

Equations (12)

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n CdSe = 1+(ε1)/[1+ (7.5/D) 1.2 ] ,
α(I)={ α 0 1+I/ I s forahomogeneousbroadeningsystem(SA1) α 0 1+I/ I s foraninhomogeneousbroadeningsystem(SA2),
T(x)=1+ 4x ( x 2 +1)( x 2 +9) Δ Φ 0 (3) + 8x ( x 2 +1) 2 ( x 2 +25) Δ Φ 0 (5) ,
Δϕ( z,r,t )=k n 2 0 L I( z ,r,t)d z +k n 4 0 L I 2 ( z ,r,t)d z ,
E e (z,r,t)= I(L) exp[iΔϕ(z,r,t)].
E a (z,r,t)= I(L) m=0 [iΔϕ(z,r=0,t)] m m! w m0 w m exp( r 2 w m 2 ik r 2 2 R m +i θ m ).
T(z)= P T (z,t)dt S P i (t)dt ,
P T (z,t)=2π 0 r a I a (z,r,t)rdr= c ε 0 n 0 π 0 r a | E a (z,r,t) | 2 rdr,
n thermal = dn dT F 0 α 0 2ρ C v I 0 ,
χ eff (3) =f|q | 2 q 2 χ n (3) ,
q= 3 ε h ε n +2 ε h ,
χ eff (5) =f|q | 4 q 2 χ n (5) .

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