Abstract

HfO2SiO2 mixed composite thin films have been deposited on fused silica substrate by co-evaporation of HfO2 and SiO2 through the reactive electron-beam evaporation technique. The composition-dependent refractive index and the absorption coefficient have been analyzed using different effective medium approximation (EMA) models in order to evaluate the suitability of these models for such mixed composite thin films. The discrepancies between experimentally determined and EMA-computed values are explained through microstructural and morphological evolutions observed in these mixed composite films. Finally, the dependence of the laser damage threshold as a function of silica content has been investigated, and the improved laser-induced damage threshold for films having more than 80% silica content has been explained through the defect-assisted multiphoton ionization process.

© 2014 Optical Society of America

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2014

H. Liu, S. Chen, P. Ma, Y. Pu, Z. Qiao, Z. Zhang, Y. Wei, and Z. Liu, “Ion beam sputtering mixture films with tailored refractive indices,” Opt. Laser Technol. 55, 21–25 (2014).
[CrossRef]

2013

S. Jena, R. B. Tokas, N. M. Kamble, S. Thakur, D. Bhattacharya, and N. K. Sahoo, “Investigation of elastic and optical properties of electron beam evaporated ZrO2-MgO composite thin films,” Thin Solid Films 537, 163–170 (2013).
[CrossRef]

M. Mende, S. Schrameyer, H. Ehlers, D. Ristau, and L. Gallais, “Laser damage resistance of ion-beam sputtered Sc2O3/SiO2 mixture optical coatings,” Appl. Opt. 52, 1368–1376 (2013).
[CrossRef]

W. Rudolph, L. A. Emmert, C. Rodriguez, Z. Sun, X. Zhang, Y. Xu, C. S. Menoni, P. F. Langston, E. Krous, and D. Patel, “Femtosecond to nanosecond laser damage in dielectric materials,” Proc. SPIE 8786, 878602 (2013).
[CrossRef]

2012

2011

2010

N. C. Das, N. K. Sahoo, D. Bhattacharyya, S. Thakur, N. M. Kamble, D. Nanda, S. Hazra, J. K. Bal, J. F. Lee, Y. L. Tai, and C. A. Hsieh, “Correlation between local structure and refractive index of e-beam evaporated (HfO2-SiO2) composite thin films,” J. Appl. Phys. 108, 023515 (2010).
[CrossRef]

2009

C. V. Ramana, R. S. Vemuri, I. Fernadez, and A. L. Campbell, “Size-effects on the optical properties of zirconium oxide thin films,” Appl. Phys. Lett. 95, 231905 (2009).
[CrossRef]

D. Ristau, M. Jupe, and K. Starke, “Laser damage thresholds of optical coatings,” Thin Solid Films 518, 1607–1613 (2009).
[CrossRef]

2008

J. Sabcho-Parramon and V. Janicki, “Effective medium theories for composite materials in spectral ranges of weak absorption: the case of Nb2O5-SiO2 mixtures,” J. Phys. D 41, 215304 (2008).
[CrossRef]

J. Sancho-Parramon, V. Janicki, and H. Zorc, “Compositional dependence of absorption coefficient and band-gap for Nb2O5-SiO2 mixture thin films,” Thin Solid Films 516, 5478–5482 (2008).
[CrossRef]

D. Nguyen, L. A. Emmert, I. V. Cravetchi, M. Mero, W. Rudolph, M. Jupe, M. Lappschies, K. Starke, and D. Ristau, “TixSi1-x O2 optical coatings with tunable index and their response to intense subpicosecond laser pulse irradiation,” Appl. Phys. Lett. 93, 261903 (2008).
[CrossRef]

J. Weber, H. Bartzch, and P. Frach, “Sputter deposition of silicon oxynitride gradient and multilayer coatings,” Appl. Opt. 47, C288–C292 (2008).
[CrossRef]

L. Gallais, J. Capoulade, J. Y. Natoli, and M. Commandre, “Investigation of nanodefect properties in optical coatings by coupling measured and simulated laser damage statistics,” J. Appl. Phys. 104, 053120 (2008).
[CrossRef]

2007

L. Gallais, J. Capoulade, F. Wagner, J. Y. Natoli, and M. Commandre, “Analysis of material modifications induced during laser damage in SiO2 thin films,” Opt. Commun. 272, 221–226 (2007).
[CrossRef]

L. Gallais, H. Krol, J. Y. Natoli, M. Commandre, and M. Cathelinaud, “Laser damage resistance of silica thin films deposited by electron beam deposition, ion assisted deposition, reactive low voltage ion plating and dual ion beam sputtering,” Thin Solid Films 515, 3830–3836 (2007).
[CrossRef]

N. K. Sahoo, A. Thakur, R. B. Tokas, and N. M. Kamble, “Refractive-index tailoring and morphological evolutions in Gd2O3–SiO2 and ZrO2–SiO2 composite thin films,” Appl. Phys. A 89, 711–719 (2007).
[CrossRef]

N. K. Sahoo, S. Thakur, R. B. Tokas, and N. M. Kamble, “Relative performances of effective medium formulations in interpreting specific composite thin films optical properties,” Appl. Surf. Sci. 253, 6787–6799 (2007).
[CrossRef]

2006

2005

L. Yang, Y. Lai, J. S. Chen, P. H. Tsai, C. L. Chen, and C. J. Chang, “Compositional tailored sol-gel SiO2–TiO2 thin films: crystallization, chemical bonding configuration, and optical properties,” J. Mater. Res. 20, 3141–3149 (2005).
[CrossRef]

G.-L. Tian, H.-B. He, and J.-D. Shao, “Effect of microstructure of TiO2 thin films on optical band gap energy,” Chin. Phys. Lett. 22, 1787–1789 (2005).
[CrossRef]

H. Krol, L. Gallais, C. Grezes-Besset, J. Y. Natoli, and M. Commandre, “Investigation of nanoprecursors threshold distribution in laser-damage testing,” Opt. Commun. 256, 184–189 (2005).
[CrossRef]

T. E. Itina, M. Mamatkulov, and M. Sentis, “Nonlinear fluence dependencies in femtosecond laser ablation of metals and dielectric materials,” Opt. Eng. 44, 051109 (2005).
[CrossRef]

2004

2003

L. Gao and Z. Li, “Effective medium approximation for two-component nonlinear composites with shape distribution,” J. Phys. Condens. Matter 15, 4397–4409 (2003).
[CrossRef]

C. W. Carr, H. B. Radousky, and S. G. Demos, “Wavelength dependence of laser-induced damage: determining the damage initiation mechanisms,” Phys. Rev. Lett. 91, 127402 (2003).
[CrossRef]

J. F. Bisson, Y. Feng, A. Shirakawa, H. Yoneda, J. Lu, H. Yagi, T. Yanagitani, and K. I. Ueda, “Laser damage threshold of ceramic YAG,” Jpn. J. Appl. Phys. 42, L1025–L1027 (2003).
[CrossRef]

2000

K. Saito and A. J. Ikushima, “Absorption edge in silica glass,” Phys. Rev. B 62, 8584–8587 (2000).
[CrossRef]

M. Alvisi, M. D. Giulio, S. G. Marrone, M. R. Perrone, M. L. Protopapa, A. Valentini, and L. Vasanelli, “HfO2 films with high laser damage threshold,” Thin Solid Films 358, 250–258 (2000).
[CrossRef]

R. Ruppin, “Evaluation of extended Maxwell-Garnett theories,” Opt. Commun. 182, 273–279 (2000).
[CrossRef]

A. Gibaud and S. Hazra, “X-ray reflectivity and diffuse scattering,” Curr. Sci. 78, 1467–1477 (2000).

M. Mulato, I. Chambouleyron, E. G. Birgin, and J. M. Martinez, “Determination of thickness and optical constants of amorphous silicon films from transmission data,” Appl. Phys. Lett. 77, 2133–2135 (2000).
[CrossRef]

1999

C. P. Wong and R. S. Bollampally, “Thermal conductivity, elastic modulus, and coefficient of thermal expansion of polymer composites filled with ceramic particles for electronic packaging,” J. Appl. Polym. Sci. 74, 3396–3403 (1999).
[CrossRef]

X. Wang, H. Masumoto, Y. Someno, and T. Hirai, “Microstructure and optical properties of amorphous TiO2-SiO2 composite films synthesized by helicon plasma sputtering,” Thin Solid Films 338, 105–109 (1999).
[CrossRef]

1998

L. Skuja, “Optically active oxygen-deficiency-related centres in amorphous silicon dioxide,” J. Non-Cryst. Solids 239, 16–48 (1998).
[CrossRef]

1996

B. C. Stuart, M. D. Feit, S. Herman, A. M. Rubenchik, B. W. Shore, and M. D. Perry, “Nanosecond-to-femtosecond laser-induced breakdown in dielectrics,” Phys. Rev. B 53, 1749–1761 (1996).
[CrossRef]

R. J. Gehr and R. W. Boyd, “Optical properties of nanostructured optical materials,” Chem. Mater. 8, 1807–1819 (1996).
[CrossRef]

J. S. Chen, S. Chao, J. S. Kao, H. Niu, and C. H. Chen, “Mixed films of TiO2–SiO2 deposited by double electron-beam coevaporation,” Appl. Opt. 35, 90–96 (1996).
[CrossRef]

1993

1989

1985

1984

L. D. Merkle, N. Koumvakalis, and M. Bass, “Laser-induced bulk damage in SiO2 at 1.064, 0.532, and 0.355 μm,” J. Appl. Phys. 55, 772–775 (1984).
[CrossRef]

1983

1982

D. E. Aspnes, “Optical properties of thin films,” Thin Solid Films 89, 249–262 (1982).
[CrossRef]

1965

H. Looyenga, “Dielectric constants of heterogeneous mixtures,” Physica 31, 401–406 (1965).
[CrossRef]

1935

D. A. G. Bruggeman, “Berechnung verschiedener physikalischer Konstanten von heterogenen Substanzen,” Ann. Phys. 416, 636–664 (1935).
[CrossRef]

1904

J. C. M. Garnett, “Colours in metal glasses and in metallic films,” Phil. Trans. R. Soc. A 203, 385–420 (1904).
[CrossRef]

1880

L. Lorentz, “Über die Refractionsconstante,” Ann. Phys. 247, 70–103 (1880).
[CrossRef]

Alvisi, M.

M. Alvisi, M. D. Giulio, S. G. Marrone, M. R. Perrone, M. L. Protopapa, A. Valentini, and L. Vasanelli, “HfO2 films with high laser damage threshold,” Thin Solid Films 358, 250–258 (2000).
[CrossRef]

Arntzen, M.

Aspnes, D. E.

D. E. Aspnes, “Optical properties of thin films,” Thin Solid Films 89, 249–262 (1982).
[CrossRef]

Bal, J. K.

N. C. Das, N. K. Sahoo, D. Bhattacharyya, S. Thakur, N. M. Kamble, D. Nanda, S. Hazra, J. K. Bal, J. F. Lee, Y. L. Tai, and C. A. Hsieh, “Correlation between local structure and refractive index of e-beam evaporated (HfO2-SiO2) composite thin films,” J. Appl. Phys. 108, 023515 (2010).
[CrossRef]

Bartzch, H.

Bass, M.

L. D. Merkle, N. Koumvakalis, and M. Bass, “Laser-induced bulk damage in SiO2 at 1.064, 0.532, and 0.355 μm,” J. Appl. Phys. 55, 772–775 (1984).
[CrossRef]

Baumgarten, B.

Bhattacharya, D.

S. Jena, R. B. Tokas, N. M. Kamble, S. Thakur, D. Bhattacharya, and N. K. Sahoo, “Investigation of elastic and optical properties of electron beam evaporated ZrO2-MgO composite thin films,” Thin Solid Films 537, 163–170 (2013).
[CrossRef]

Bhattacharyya, D.

N. C. Das, N. K. Sahoo, D. Bhattacharyya, S. Thakur, N. M. Kamble, D. Nanda, S. Hazra, J. K. Bal, J. F. Lee, Y. L. Tai, and C. A. Hsieh, “Correlation between local structure and refractive index of e-beam evaporated (HfO2-SiO2) composite thin films,” J. Appl. Phys. 108, 023515 (2010).
[CrossRef]

Birgin, E. G.

M. Mulato, I. Chambouleyron, E. G. Birgin, and J. M. Martinez, “Determination of thickness and optical constants of amorphous silicon films from transmission data,” Appl. Phys. Lett. 77, 2133–2135 (2000).
[CrossRef]

Bischoff, M.

Bisson, J. F.

J. F. Bisson, Y. Feng, A. Shirakawa, H. Yoneda, J. Lu, H. Yagi, T. Yanagitani, and K. I. Ueda, “Laser damage threshold of ceramic YAG,” Jpn. J. Appl. Phys. 42, L1025–L1027 (2003).
[CrossRef]

Bollampally, R. S.

C. P. Wong and R. S. Bollampally, “Thermal conductivity, elastic modulus, and coefficient of thermal expansion of polymer composites filled with ceramic particles for electronic packaging,” J. Appl. Polym. Sci. 74, 3396–3403 (1999).
[CrossRef]

Boyd, R. W.

R. J. Gehr and R. W. Boyd, “Optical properties of nanostructured optical materials,” Chem. Mater. 8, 1807–1819 (1996).
[CrossRef]

Brauer, G.

Bruggeman, D. A. G.

D. A. G. Bruggeman, “Berechnung verschiedener physikalischer Konstanten von heterogenen Substanzen,” Ann. Phys. 416, 636–664 (1935).
[CrossRef]

Bruns, S.

Burdack, P.

Burns, S. J.

Campbell, A. L.

C. V. Ramana, R. S. Vemuri, I. Fernadez, and A. L. Campbell, “Size-effects on the optical properties of zirconium oxide thin films,” Appl. Phys. Lett. 95, 231905 (2009).
[CrossRef]

Capoulade, J.

L. Gallais, J. Capoulade, J. Y. Natoli, and M. Commandre, “Investigation of nanodefect properties in optical coatings by coupling measured and simulated laser damage statistics,” J. Appl. Phys. 104, 053120 (2008).
[CrossRef]

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Figures (13)

Fig. 1.
Fig. 1.

Transmission and reflection of HfO2SiO2 mixed composite thin films.

Fig. 2.
Fig. 2.

Experimental transmission with best-fit theoretical simulation of HfO2(90%)-SiO2(10%) mixed film.

Fig. 3.
Fig. 3.

Refractive index spectra of HfO2SiO2 mixed thin films.

Fig. 4.
Fig. 4.

Dispersion of absorption coefficient for HfO2SiO2 mixed thin films.

Fig. 5.
Fig. 5.

Plot of (αhν)1/2 versus hν for HfO2SiO2 mixed thin films.

Fig. 6.
Fig. 6.

Experimental x-ray reflectivity with best-fit theoretical simulation for pure HfO2 and HfO2(90%)-SiO2(10%) mixed film.

Fig. 7.
Fig. 7.

Surface morphology of representative HfO2SiO2 mixed composite thin films.

Fig. 8.
Fig. 8.

Schematic diagram of laser-induced damage threshold (LIDT) measurement setup.

Fig. 9.
Fig. 9.

Comparison of experimental and computed effective refractive index at 266 and 532 nm using different EMA models for HfO2SiO2 mixed thin films.

Fig. 10.
Fig. 10.

Comparison of experimental and computed effective absorption coefficient at 5.82 and 6.42 eV using different EMA models for HfO2SiO2 mixed thin films.

Fig. 11.
Fig. 11.

Laser-induced damage threshold (LIDT) for HfO2SiO2 mixed thin films and LIDT versus bandgap (inset plot).

Fig. 12.
Fig. 12.

Internal stress as a function of % SiO2 in HfO2SiO2 mixed composite thin films.

Fig. 13.
Fig. 13.

Laser-induced damage morphology of HfO2SiO2 mixed composite thin films.

Tables (1)

Tables Icon

Table 1. Parameters Obtained from Transmission, GIXR, AFM, and LIDT Measurement of HfO2SiO2 Films and Fused Silica Substrate

Equations (10)

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

αfilm(λ)=1dfilmln(1RT/Tsub),
fε1εeffε1+2εeff+(1f)ε2εeffε2+2εeff=0,
εeffε2εeff+2ε2=fε1ε2ε1+2ε2,
εeff1εeff+2=fε11ε1+2+(1f)ε21ε2+2,
εeff=fε1+(1f)ε2,
εeff1/2=fε11/2+(1f)ε21/2,
εeff1/3=fε11/3+(1f)ε21/3,
ΔPALαCEρ,
dNedt=Nσ(n)(I/hν)n,
Ic=(Ne(Nσ(3)τ)3)E,

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