Enhanced band structure, optoelectronic and magnetic properties of spray pyrolysis Ni-doped SnO2 nanostructured films

doi:10.1016/j.matchemphys.2020.122892

Materials Chemistry and Physics

Volume 248, 1 July 2020, 122892

https://doi.org/10.1016/j.matchemphys.2020.122892 Get rights and content

Highlights

•
Ni-doped SnO₂ nanocrystalline thin films were synthesized by home-made Spray Pyrolysis method.
•
The films have been investigated structurally, morphologically, optically and magnetically.
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The enhancement in the band structure is observed due to the increasing of the Ni in the SnO₂ lattice.
•
The dispersion and single oscillator parameters of the films were determined.
•
Room temperature ferromagnetism is observed which is attributed to BMP model.

Abstract

Pure and Nickel-doped Tin Oxide at 0, 1, 2, 4, 5, 6, and 7 wt % of Ni nanocrystalline thin films were synthesized by home-made Spray Pyrolysis technique on glass substrate. The microstructural, morphological, optical and magnetic properties of the films have been investigated. The XRD patterns of the films exhibit a tetragonal type structure with no signature of extra phases. The solubility limit of the incorporation of Ni into the SnO₂ semiconducting matrix has been observed at x > 0.05. The nanocrystalline feature of the films is confirmed from AFM and SEM investigations. It was found that the optical energy gap E_g diminishes with the increasing of Ni content up to x ≤ 0.05 and then increases due to the solubility limit of Ni, suggesting the enhancement in the band structure. The decrease of the optical band gap could be attributed to the sp-d exchange interaction while the increase of E_g is explained according to the Burstein–Moss effect. The dispersion and single oscillator parameters of the films were estimated by analyzing the dispersion data based on Wemple–DiDomenico single-effective-oscillator model. The room temperature ferromagnetic behaviour of the films has been observed and discussed according to the bound magnetic polarons model.

Introduction

Integrating spin functionality into nonmangnetic semiconductor has opened up a route for developing multifunctional applications like spintronics and optoelectronics devices [[1], [2], [3], [4]]. Towards this end, early attempts in recent years for the synthesis of diluted magnetic semiconductors (DMSs) have been attained, where the transition metals e.g. Cr, Mn, Co, Ni doped into nomagnetic semiconductor (III–V and II-VI compounds). Furthermore, DMSs reveal ferromagnetic [1,5,6], optoelectronic [[7], [8], [9], [10]], and spin glass behavior [11]. The presence of ferromagnetism at and/or above room temperature in TM-doped DMSs has been investigated [12,13]. On the other hand, the observation of high Curie temperature in Co-doped TiO₂ and the room temperature ferromagnetism in TiO₂, ZnO, In₂O₃, SnO₂, suggests that the diluted magnetic oxide semiconductors (DMOS) are interesting materials for spintronic applications [14]. Among various oxide semiconductors, Tin oxide (SnO₂) is reported to be attractive oxide semiconductor with special features such as wide optical band gap of 3.6 eV, native oxygen vacancies, higher carrier density, higher optical transparency, higher electrical conductivity and higher chemical stability. Its interesting properties provide suitable material for solar cells, gas sensors, and optoelectronic applications. Nowadays, many reports were revealed the high temperature ferromagnetism in transition metals doped SnO₂ nanostructure such as Fe [14,15], Co [16], Mn [[17], [18], [19]], and Ni [[20], [21], [22], [23], [24], [25], [26]]. The photo electrochemical results of Sb doped SnO₂ films prepared by spray technique reported by Y. Bouznit and A. Henni [27] showed clearly that the ability of SnO₂:Sb nanostructured to generate significant photocurrents under UV light and the films suitable for application in photo electrochemical implications.

It well known that Ni²⁺ ions can be introduced into the SnO₂ lattice to increase the carrier concentration of the samples and origins an imbalance in the total valence state of the compound, hence may considered to be noble applicant for doping to induce ferromagnetism in the samples [28]. Thus, various experimental investigations on the magnetic and structural properties of Ni doped SnO₂ nanoparticles and/or films have been reported [[20], [21], [22], [23], [24], [25], [26]]. The large electronegativity of oxygen is suggested to present strong p-d exchange coupling between localized spins and band carriers [21,26,29]. However, the magnetic moments of the DMOS depend intensely on preparation methods and there is still no certain conclusion for the source of the nature of magnetism of DMSs [30]. Therefore, many methods, such as pulsed laser deposition [21,23,24], hydrothermal [31], solid state reaction [32], sol-gel [33], co-precipitation method [34,35], have been specified for the synthesis of Ni-doped SnO₂. Several groups have showed room temperature ferromagnetism in Mn- doped SnO₂ thin films [17,18] and nanocrystals [19]. The observed ferromagnetism is reported to be caused by the formation of impurity phases or clustering of magnetic metals in the synthesized compounds [17,18]. Furthermore, nanocrystalline sample of Mn, Ni doped tin oxide have been reported to be ferromagnetic [18], however, other group have been reported to be paramagnetic [36]. It was reported that the magnetic behaviour of the Ni-doped SnO₂ films/and or nanoparticles annealed under N₂ atmosphere changed from paramagnetic to ferromagnetic with magnetic moment increases significantly with the increasing of the annealing time [20,22] Besides, Hong et al. [37] reported that the formation of the ferromagnetism in Ni doped SnO₂ is govern by the oxygen vacancies (V_o). Additionally, the first-principles density functional calculations have been performed by Wang el al [38]. in order to study the effects of Ni doping and V_o on the electronic and magnetic properties of Ni-doped SnO₂ samples. The obtained results show that the samples are nonmagnetic without V_o, while V_o induces magnetic moments. Nevertheless, studies of the magnetic and optoelectronic properties of Ni-doped SnO₂ films synthesized by spray pyrolysis technique are relatively rare. Hence, in this work an effort was performed to produce nanostructure Ni-doped SnO₂ films by home-made spray pyrolysis method with different doping contents to investigate the optoelectronic and magnetic properties upon the effect of Ni doping in the SnO₂ host semiconductor matrix. The morphological and microstructural properties were also studied.

Section snippets

Synthesis of spray pyrolysis thin films

Nanocrystalline Sn_1-x Ni_xO₂ films with various Ni concentrations (x = 0.00, 0.01, 0.02, 0.04, 0.05, 0.06 and 0.07) were synthesized by home-made spray pyrolysis technique which is defined as SnO₂: Ni at 0, 1, 2, 4, 5, 6 and 7 wt %). The precursor compounds of SnCl₂.2H₂O and NiCl₂.6H₂O with purity greater than 97%, Oxford Co., INDIA were used. Initially, the precursor solutions of un-doped and Ni-doped SnO₂ with different doping concentrations were prepared by dissolving (0.2 M) of SnCl₂.2H₂O

Compositional analysis

The EDXS analysis of the spray pyrolysis Sn_1-x Ni_xO₂ films (x = 0.02–0.05) shown in Fig. 2, confirming the presence of Tin, Nickel and oxygen with approximately stoichiometric amount, which emphasize further the absence of any impurity elements in the prepared samples. The extra peaks displayed in the EDX spectra other than Sn, Ni and O peaks are due to constitutes of the glass substrate such as Si, Mg and P etc.

Structural and microstructural investigation

Fig. 3 (a) displays the XRD spectra of the spray pyrolysis Sn_1-xNi_xO₂ films with

Summary

To summarize, we presented the investigation on the microstructure, morphology, topology, optical, and magnetic properties of the nanocrystalline Ni-doped Tin Oxide films synthesized by home-made Spray Pyrolysis method on glass substrate. The films structurally reveal a tetragonal type structure. The morphologically images confirm the nanostructure behaviour of the films. The enhancement in the band structure was observed which is attributed to the increasing of Ni content and discussed

CRediT authorship contribution statement

M.I. Amer: Software, Validation, Writing - original draft. S.H. Moustafa: Investigation, Formal analysis, Visualization, Resources, Validation. M. El-Hagary: Conceptualization, Methodology, Data curation, Writing - review & editing, Project administration.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

This work was supported by Science & Technology Development Fund, Ministry of Scientific Research, STDF, Egypt under grant “Basic & Applied Research” No. 15027. The contribution of Dr. Hany Hashem, physics department Faculty of Science, Helwan University, during the experimental work is acknowledged.

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Citation Excerpt :
This means that there is a tensile microstrain embedded in the SnO2 lattice. These practical observations follow the reported results of Mn-doped SnO2 [30] and Ni-doped SnO2 [31]. The morphology of nanocrystalline films prepared by different deposition techniques has been extensively investigated to accurately study the surface structure.
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Enhanced band structure, optoelectronic and magnetic properties of spray pyrolysis Ni-doped SnO2 nanostructured films

Highlights

Abstract

Introduction

Section snippets

Synthesis of spray pyrolysis thin films

Compositional analysis

Structural and microstructural investigation

Summary

CRediT authorship contribution statement

Declaration of competing interest

Acknowledgments

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Low-temperature activation and deactivation of high-curie-temperature ferromagnetism in a new diluted magnetic Semiconductor: Ni2+-doped SnO2

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Enhanced band structure, optoelectronic and magnetic properties of spray pyrolysis Ni-doped SnO₂ nanostructured films

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Structural and optical investigation of nanocrystalline Zn_1−xNi_xS diluted magnetic semiconductor thin films

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