Investigation on the optical properties of annealed Mn-Co-Ni-O thin films by spectroscopic ellipsometry

Wei Zhou; Yi Liu; Yimin Yin; Wanli Ma; Zhiming Huang

doi:10.1364/OL.44.002701

Optics Letters
Vol. 44,
Issue 11,
pp. 2701-2704
(2019)
•https://doi.org/10.1364/OL.44.002701

Investigation on the optical properties of annealed Mn-Co-Ni-O thin films by spectroscopic ellipsometry

Wei Zhou, Yi Liu, Yimin Yin, Wanli Ma, and Zhiming Huang

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Wei Zhou, Yi Liu, Yimin Yin, Wanli Ma, and Zhiming Huang, "Investigation on the optical properties of annealed Mn-Co-Ni-O thin films by spectroscopic ellipsometry," Opt. Lett. 44, 2701-2704 (2019)

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Abstract

Mn-Co-Ni-O thin films have been widely used for their excellent negative temperature coefficient features, but investigations about tailoring their structural and optical properties via a post-annealing (PA) process are still rare in recent years. In this Letter, we derived the visible to near-infrared optical constants of annealed ${Mn}_{1.56} {Co}_{0.96} {Ni}_{0.48} O_{4}$ (MCNO) films, and we elucidate the absorption mechanism of MCNO films by investigating the microstructure and cation distribution properties. We found that proper PA temperature will result in improved crystallinity, balanced distribution of ${Mn}^{3 +}$ and ${Mn}^{4 +}$ ions, and larger small polaron absorption. We also revealed that it is mainly the small polaron hopping, together with the charge transfer (CT) transition process involving ${Co}^{2 +}$ and $O^{2 -}$ cations, which contributes to the absorption at 750 to 1100 nm. The process of ${Mn}^{3 +}$ occupying the octahedral sites reduces the concentration of ${Co}^{2 +}$ and the absorption peak at 1.3 eV. This Letter will improve the mechanism study of small polaron hopping and CT absorption for MCNO films, which is important to the development of optoelectronic devices based on transition metal oxides.

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	S1 (450 °C)	S2 (600 °C)	S3 (750 °C)
$R_{a}$	0.58 nm	3.25 nm	7.74 nm
$R_{rms}$	0.72 nm	4.22 nm	9.63 nm

	${Mn}^{2 +}$	${Mn}^{3 +}$	${Mn}^{4 +}$	Nc(1-c)	Formula
450°C	51.2%	31.4%	17.4%	0.112	${({Co}_{0.15}^{2 +} {Mn}_{0.85}^{2 +})}_{T} {[{Ni}_{0.48}^{2 +} {Co}_{0.81}^{2 +} {Mn}_{0.41}^{3 +} {Mn}_{0.30}^{4 +}]}_{O} O_{3.51}^{2 -}$
600°C	47.3%	18.2%	34.5%	0.120	${({Co}_{0.26}^{2 +} {Mn}_{0.74}^{2 +})}_{T} {[{Ni}_{0.48}^{2 +} {Co}_{0.70}^{2 +} {Mn}_{0.28}^{3 +} {Mn}_{0.54}^{4 +}]}_{O} O_{3.68}^{2 -}$
750°C	17.3%	37.2%	45.5%	0.205	${({Co}_{0.73}^{2 +} {Mn}_{0.27}^{2 +})}_{T} {[{Ni}_{0.48}^{2 +} {Co}_{0.27}^{2 +} {Mn}_{0.58}^{3 +} {Mn}_{0.71}^{4 +}]}_{O} O_{4.04}^{2 -}$

		450°C	600°C	750°C
Tauc–Lorentz-1TL1	Amp	7.004	12.13	16.96
	En	1.84	1.92	2.05
	C	0.826	3.22	1.44
	Eg	1.737	1.418	1.709
Tauc–Lorentz-2TL2	Amp	9.51	9.93	4.32
	En	1.38	1.35	1.65
	C	0.319	0.768	1.06
	Eg	1.213	1.022	0.607
Lorentz-1L1	Amp	1.688	3.119	3.380
	Br	10	8.87	10
	En	6.39	9.50	8.36
Lorentz-2L2	Amp		2.449	1.036
	Br		0.220	0.265
	En		1.247	1.341

	S1 (450 °C)	S2 (600 °C)	S3 (750 °C)
$R_{a}$	0.58 nm	3.25 nm	7.74 nm
$R_{rms}$	0.72 nm	4.22 nm	9.63 nm

	${Mn}^{2 +}$	${Mn}^{3 +}$	${Mn}^{4 +}$	Nc(1-c)	Formula
450°C	51.2%	31.4%	17.4%	0.112	${({Co}_{0.15}^{2 +} {Mn}_{0.85}^{2 +})}_{T} {[{Ni}_{0.48}^{2 +} {Co}_{0.81}^{2 +} {Mn}_{0.41}^{3 +} {Mn}_{0.30}^{4 +}]}_{O} O_{3.51}^{2 -}$
600°C	47.3%	18.2%	34.5%	0.120	${({Co}_{0.26}^{2 +} {Mn}_{0.74}^{2 +})}_{T} {[{Ni}_{0.48}^{2 +} {Co}_{0.70}^{2 +} {Mn}_{0.28}^{3 +} {Mn}_{0.54}^{4 +}]}_{O} O_{3.68}^{2 -}$
750°C	17.3%	37.2%	45.5%	0.205	${({Co}_{0.73}^{2 +} {Mn}_{0.27}^{2 +})}_{T} {[{Ni}_{0.48}^{2 +} {Co}_{0.27}^{2 +} {Mn}_{0.58}^{3 +} {Mn}_{0.71}^{4 +}]}_{O} O_{4.04}^{2 -}$

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Optics Letters