Abstract

A great deal of intensive research has been conducted to obtain high-quality transparent ultralow-refractive-index and ultralow-dielectric-constant thin films for microptics and microelectronics applications. Here, we report a simple procedure to prepare highly porous silica thin films with high optical quality and water resistance through nano-etching of mesoporous silica films followed by fluoroalkylsilane surface modification. The films possess an ultralow refractive index of 1.03 (800 nm) and an ultralow dielectric constant of 1.30 (100 kHz), to our knowledge the lowest values ever reported in thin film materials. The films are superhydrophobic (water contact angle=156deg), thus exhibit high moisture stability.

© 2012 Optical Society of America

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F. Chi, L. Yan, H. Lv, and B. Jiang, Mater. Lett. 65, 1095 (2011).
[CrossRef]

2010

Y. Du, L. E. Luna, W. S. Tan, M. F. Rubner, and R. E. Cohen, ACS Nano 4, 4308 (2010).
[CrossRef]

2009

2007

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

E. F. Schubert, J. K. Kim, and J.-Q. Xi, Phys. Status Solidi B 244, 3002(2007).
[CrossRef]

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

D. Grosso, C. Boissiére, and C. Sanchez, Nat. Mat. 6, 572 (2007).
[CrossRef]

2006

T. Baldacchini, J. E. Carey, M. Zhou, and E. Mazur, Langmuir 22, 4917 (2006).
[CrossRef]

J.-Q. Xi, J. K. Kim, E. F. Schubert, D. Ye, T.-M. Lu, and S.-Y. Lin, Opt. Lett. 31, 601 (2006).
[CrossRef]

2005

J.-Q. Xi, M. Ojha, W. Cho, J. L. Plawsky, and W. N. Gill, Opt. Lett. 30, 1518 (2005).
[CrossRef]

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

1998

S. Inagaki and Y. Fukushima, Microporous Mesoporous Mater. 21, 667 (1998).
[CrossRef]

Baldacchini, T.

T. Baldacchini, J. E. Carey, M. Zhou, and E. Mazur, Langmuir 22, 4917 (2006).
[CrossRef]

Bo, J.

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

Boissiere, C.

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

Boissiére, C.

D. Grosso, C. Boissiére, and C. Sanchez, Nat. Mat. 6, 572 (2007).
[CrossRef]

Bruneau, A. B.

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

Carey, J. E.

T. Baldacchini, J. E. Carey, M. Zhou, and E. Mazur, Langmuir 22, 4917 (2006).
[CrossRef]

Chen, M.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

Chi, F.

F. Chi, L. Yan, H. Lv, and B. Jiang, Mater. Lett. 65, 1095 (2011).
[CrossRef]

Cho, W.

Cohen, R. E.

Y. Du, L. E. Luna, W. S. Tan, M. F. Rubner, and R. E. Cohen, ACS Nano 4, 4308 (2010).
[CrossRef]

Du, Y.

Y. Du, L. E. Luna, W. S. Tan, M. F. Rubner, and R. E. Cohen, ACS Nano 4, 4308 (2010).
[CrossRef]

F.-Ting, C.

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

Fukushima, Y.

S. Inagaki and Y. Fukushima, Microporous Mesoporous Mater. 21, 667 (1998).
[CrossRef]

Gill, W. N.

Grosso, D.

D. Grosso, C. Boissiére, and C. Sanchez, Nat. Mat. 6, 572 (2007).
[CrossRef]

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

Hai-Bing, L.

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

Hong, Y.-L.

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

Imai, H.

Inagaki, S.

S. Inagaki and Y. Fukushima, Microporous Mesoporous Mater. 21, 667 (1998).
[CrossRef]

Jiang, B.

F. Chi, L. Yan, H. Lv, and B. Jiang, Mater. Lett. 65, 1095 (2011).
[CrossRef]

Kim, J. K.

E. F. Schubert, J. K. Kim, and J.-Q. Xi, Phys. Status Solidi B 244, 3002(2007).
[CrossRef]

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

J.-Q. Xi, J. K. Kim, E. F. Schubert, D. Ye, T.-M. Lu, and S.-Y. Lin, Opt. Lett. 31, 601 (2006).
[CrossRef]

Lepoutre, S.

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

Lin, S.-Y.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

J.-Q. Xi, J. K. Kim, E. F. Schubert, D. Ye, T.-M. Lu, and S.-Y. Lin, Opt. Lett. 31, 601 (2006).
[CrossRef]

Liu, W.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

Lu, T.-M.

Luna, L. E.

Y. Du, L. E. Luna, W. S. Tan, M. F. Rubner, and R. E. Cohen, ACS Nano 4, 4308 (2010).
[CrossRef]

Lv, H.

F. Chi, L. Yan, H. Lv, and B. Jiang, Mater. Lett. 65, 1095 (2011).
[CrossRef]

Mazur, E.

T. Baldacchini, J. E. Carey, M. Zhou, and E. Mazur, Langmuir 22, 4917 (2006).
[CrossRef]

Nakayama, H.

Nicole, L.

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

Ojha, M.

Plawsky, J. L.

Rubner, M. F.

Y. Du, L. E. Luna, W. S. Tan, M. F. Rubner, and R. E. Cohen, ACS Nano 4, 4308 (2010).
[CrossRef]

Sanchez, C.

D. Grosso, C. Boissiére, and C. Sanchez, Nat. Mat. 6, 572 (2007).
[CrossRef]

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

Schubert, E. F.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

E. F. Schubert, J. K. Kim, and J.-Q. Xi, Phys. Status Solidi B 244, 3002(2007).
[CrossRef]

J.-Q. Xi, J. K. Kim, E. F. Schubert, D. Ye, T.-M. Lu, and S.-Y. Lin, Opt. Lett. 31, 601 (2006).
[CrossRef]

Schubert, M. F.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

Smart, J. A.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

Tan, W. S.

Y. Du, L. E. Luna, W. S. Tan, M. F. Rubner, and R. E. Cohen, ACS Nano 4, 4308 (2010).
[CrossRef]

Xi, J.-Q.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

E. F. Schubert, J. K. Kim, and J.-Q. Xi, Phys. Status Solidi B 244, 3002(2007).
[CrossRef]

J.-Q. Xi, J. K. Kim, E. F. Schubert, D. Ye, T.-M. Lu, and S.-Y. Lin, Opt. Lett. 31, 601 (2006).
[CrossRef]

J.-Q. Xi, M. Ojha, W. Cho, J. L. Plawsky, and W. N. Gill, Opt. Lett. 30, 1518 (2005).
[CrossRef]

Xiao-Dong, J.

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

Xiao-Dong, Y.

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

Yamada, K.

Yamaguchi, M.

Yan, L.

F. Chi, L. Yan, H. Lv, and B. Jiang, Mater. Lett. 65, 1095 (2011).
[CrossRef]

Ye, D.

Zhou, M.

T. Baldacchini, J. E. Carey, M. Zhou, and E. Mazur, Langmuir 22, 4917 (2006).
[CrossRef]

ACS Nano

Y. Du, L. E. Luna, W. S. Tan, M. F. Rubner, and R. E. Cohen, ACS Nano 4, 4308 (2010).
[CrossRef]

J. Inorg. Mat.

Y.-L. Hong, C. F.-Ting, J. Xiao-Dong, L. Hai-Bing, Y. Xiao-Dong, and J. Bo, J. Inorg. Mat. 22, 1247 (2007).

Langmuir

T. Baldacchini, J. E. Carey, M. Zhou, and E. Mazur, Langmuir 22, 4917 (2006).
[CrossRef]

C. Boissiere, D. Grosso, S. Lepoutre, L. Nicole, A. B. Bruneau, and C. Sanchez, Langmuir 21, 12362 (2005).
[CrossRef]

Mater. Lett.

F. Chi, L. Yan, H. Lv, and B. Jiang, Mater. Lett. 65, 1095 (2011).
[CrossRef]

Microporous Mesoporous Mater.

S. Inagaki and Y. Fukushima, Microporous Mesoporous Mater. 21, 667 (1998).
[CrossRef]

Nat. Mat.

D. Grosso, C. Boissiére, and C. Sanchez, Nat. Mat. 6, 572 (2007).
[CrossRef]

Nat. Photon.

J.-Q. Xi, M. F. Schubert, J. K. Kim, E. F. Schubert, M. Chen, S.-Y. Lin, W. Liu, and J. A. Smart, Nat. Photon. 1, 176 (2007).

Opt. Lett.

Phys. Status Solidi B

E. F. Schubert, J. K. Kim, and J.-Q. Xi, Phys. Status Solidi B 244, 3002(2007).
[CrossRef]

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Figures (5)

Fig. 1.
Fig. 1.

Experimental procedure for forming the superhydrophic ultralow-refractive-index films.

Fig. 2.
Fig. 2.

The refractive index, measured in ambient environment, and the corresponding porosity of thin films with varying ratios of F127 to TEOS as function of F127 content after annealing at 450 °C for 1 h.

Fig. 3.
Fig. 3.

The refractive index, measured in ambient condition, and the corresponding porosity of thin films with varying etching period as function of etching time. The HF concentration is 0.00001 molar.

Fig. 4.
Fig. 4.

The refractive indice of ultralow-n films FAS treated and untreated as a function of the exposure time in the humid condition. The ambient aging condition is about 20 °C and 90% relative humidity.

Fig. 5.
Fig. 5.

Schematic representation of the preparation of ultralow-refractive-index optical thin films.

Equations (1)

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porosity=1n21nd21,

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