Giant dispersive and absorptive optical nonlinearities in TiO<sub>2</sub> thin films

Romita Chouhan; Mukul Gupta; P. K. Sen; Pratima Sen

doi:10.1364/JOSAB.377851

Journal of the Optical Society of America B
Vol. 37,
Issue 2,
pp. 279-286
(2020)
•https://doi.org/10.1364/JOSAB.377851

Giant dispersive and absorptive optical nonlinearities in TiO₂ thin films

Romita Chouhan, Mukul Gupta, P. K. Sen, and Pratima Sen

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Romita Chouhan, Mukul Gupta, P. K. Sen, and Pratima Sen, "Giant dispersive and absorptive optical nonlinearities in TiO₂ thin films," J. Opt. Soc. Am. B 37, 279-286 (2020)

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Table of Contents Category
- Nonlinear or High Field Optics
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About this Article
History
- Original Manuscript: September 16, 2019
- Revised Manuscript: December 6, 2019
- Manuscript Accepted: December 6, 2019
- Published: January 14, 2020

Abstract

We report the experimental observation of giant dispersive and absorptive optical nonlinearities in direct current magnetron sputtered as-grown and annealed $ {{\rm TiO}_2} $ thin films. The $ {{\rm TiO}_2} $ film was deposited in a mixture of argon and oxygen. The as-grown film and the film annealed below 250°C demonstrated amorphous behavior having particle size variation in the range of 15–20 nm, while the films annealed above temperature $ \ge 300^\circ{\rm C} $ exhibited crystalline structure with larger particle size (50–80 nm). The enhancement in optical nonlinearity in amorphous films can be attributed to small particle sizes, while in crystalline thin films, the enhancement in optical nonlinearity is attributed to phonon-assisted resonant transitions. The films are characterized by the x-ray diffraction technique, atomic force microscopy, UV–visible spectroscopy, and Raman spectroscopy for their structural properties, morphology, bandgap, and presence of phonon modes, respectively. The intensity-dependent nonlinear optical properties of the films are analyzed by using the Z-scan technique.

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Parameters	S1	S2	S3	S4	S5
$E_{g}$ (eV)	3.19	3.19	3.08	3.17	3.13
$β \times 10^{- 2} (m / W)$	1.70	2.10	1.49	1.79	4.49
$n_{2} \times 10^{- 9} (m^{2} / W)$	−10.8	−21.70	6.57	−4.80	−33.10
$n_{4} \times 10^{- 15} (m^{4} / W^{2})$	6.58	7.20	−3.33	2.73	12.10
$n_{n l, e f f} \times 10^{- 8} (m^{2} / W)$	5.76	5.29	−2.86	2.36	9.27
$χ_{R}^{(3)} \times 10^{- 10} (m^{2} / V^{2})$	3.29	$2.98$	−1.18	0.92	3.74
$χ_{I}^{(3)} \times 10^{- 12} (m^{2} / V^{2})$	7.30	8.86	6.49	7.37	18.81
$W$	1.36	1.75	0.51	3.21	3.77
$T^{- 1}$	5.35	3.98	3.03	2.08	3.26

Sample	Laser	$χ_{R}^{(3)}$ (in esu)	$χ_{I}^{(3)}$ (in esu)	References
${T i O}_{2}$ (pure anatase film)	800 nm (50 ps)	$- 7 \times 10^{- 11}$	$- 4 \times 10^{- 11}$	Long et al. [1]
${T i O}_{2}$ (pure rutile film)	800 nm (50 ps)	$- 4 \times 10^{- 11}$	$- 2 \times 10^{- 11}$	Long et al. [1]
${T i O}_{2}$ (pure anatase film)	1900 nm (ns)	$9 \times 10^{- 13}$	—	Hashimoto et al. [2]
${T i O}_{2}$ (pure rutile film)	1900 nm (ns)	$1.4 \times 10^{- 12}$	—	Hashimoto et al. [2]
${T i O}_{2}$ (nanoporous layer)	1064 nm (42 ps)	$2 \times 10^{- 5}$	—	Gayvornsky et al. [4]
Au: ${T i O}_{2}$	DFWM $\approx 680 n m$	$6 \times 10^{- 7}$	—	Liao et al. [21]
${T i O}_{2}$	632 nm (CW He–Ne)	$\approx 10^{- 3}$	$\approx 10^{- 4}$	our work

Parameters	S1	S2	S3	S4	S5
$E_{g}$ (eV)	3.19	3.19	3.08	3.17	3.13
$β \times 10^{- 2} (m / W)$	1.70	2.10	1.49	1.79	4.49
$n_{2} \times 10^{- 9} (m^{2} / W)$	−10.8	−21.70	6.57	−4.80	−33.10
$n_{4} \times 10^{- 15} (m^{4} / W^{2})$	6.58	7.20	−3.33	2.73	12.10
$n_{n l, e f f} \times 10^{- 8} (m^{2} / W)$	5.76	5.29	−2.86	2.36	9.27
$χ_{R}^{(3)} \times 10^{- 10} (m^{2} / V^{2})$	3.29	$2.98$	−1.18	0.92	3.74
$χ_{I}^{(3)} \times 10^{- 12} (m^{2} / V^{2})$	7.30	8.86	6.49	7.37	18.81
$W$	1.36	1.75	0.51	3.21	3.77
$T^{- 1}$	5.35	3.98	3.03	2.08	3.26

Sample	Laser	$χ_{R}^{(3)}$ (in esu)	$χ_{I}^{(3)}$ (in esu)	References
${T i O}_{2}$ (pure anatase film)	800 nm (50 ps)	$- 7 \times 10^{- 11}$	$- 4 \times 10^{- 11}$	Long et al. [1]
${T i O}_{2}$ (pure rutile film)	800 nm (50 ps)	$- 4 \times 10^{- 11}$	$- 2 \times 10^{- 11}$	Long et al. [1]
${T i O}_{2}$ (pure anatase film)	1900 nm (ns)	$9 \times 10^{- 13}$	—	Hashimoto et al. [2]
${T i O}_{2}$ (pure rutile film)	1900 nm (ns)	$1.4 \times 10^{- 12}$	—	Hashimoto et al. [2]
${T i O}_{2}$ (nanoporous layer)	1064 nm (42 ps)	$2 \times 10^{- 5}$	—	Gayvornsky et al. [4]
Au: ${T i O}_{2}$	DFWM $\approx 680 n m$	$6 \times 10^{- 7}$	—	Liao et al. [21]
${T i O}_{2}$	632 nm (CW He–Ne)	$\approx 10^{- 3}$	$\approx 10^{- 4}$	our work

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Journal of the Optical Society of America B