Characterization of Fe2O3 doping on structure, optical and luminescence properties of magnesium aluminosilicate-based glasses

https://doi.org/10.1016/j.jnoncrysol.2021.120786Get rights and content

Highlights

  • Fe2O3 doped MgO-Al2O3-SiO2-B2O3 glasses are prepared and characterized.

  • The addition of Fe2O3 decreases the stability and forming ability of glass.

  • Emission spectrum and lifetime of Fe3+ ions in the glass are tested.

  • Glass obtained can be a potential candidate for the blue LED devices.

Abstract

The Fe2O3-doped magnesium aluminosilicate-based glasses were prepared by the traditional melt quenching method. The effects of Fe2O3 on the structure and properties of the prepared glasses were analyzed. DSC results indicate that the crystallization peak temperature is increasing first and then decreasing with Fe2O3 doping, and the thermal stability gradually decreases. Infrared spectrum curve illustrates that with increasing Fe2O3 content, the glass network is destroyed, and the number of non-bridging oxygen increases, resulting in a decrease of the optical band gap energy and an increase of the Urbach energy. In ultraviolet-visible absorption spectra, two bands observed around 540 and 1035 nm are corresponded to the electronic transitions of Fe3+ from 6A1g to 4T2g and Fe2+ from 5T2g to 5Eg, respectively. The obtained chromaticity coordinate parameters indicate that the prepared Fe2O3-doped magnesium aluminosilicate-based glasses can be applied to the fluorescent material of the light conversion layer of blue light-emitting diode device.

Introduction

In recent years, with the continuous integration of optics, electronic information science, and new material science, optical glass acting as the basic material of optoelectronics has a wide range of applications in military and civilian fields. Especially, the optical glass materials can be applied in tunable solid-state lasers and luminescence materials for its high permeability in the visible region [1], [2], [3], [4]. In generally, the optical glass with excellent performance can be obtained by adding some modifiers such as alkali metals, alkaline earth metals, rare earth, and transition metal oxides [5, 6]. Due to the unique electronic layer structure, transition metal oxides are widely used in various glasses to improve their structure and properties, especially the optical and fluorescent properties of glass. For instance, Mohamed et al. [7] reported the effects of transition metal oxides (such as NiO, CuO, CoO, Bi2O3) on the optical and electrical properties of 60PbO-20Bi2O3–20MxOy mol% (MxOy = B2O3 or SiO2 or P2O5) glasses. They found that the introduction of the transition metal oxide reduced the width of the bandgap in the energy band structure, making the glass transition from an insulator to a semiconductor. Also, Bates used the coordination field theory for the first time to systematically study the absorption spectra of transition metal ions-doped silicate glasses [8]. The results showed that the coordination field can be changed by adjusting the glass matrix, thereby reducing the polarization effect of oxygen ion groups on the transition metal ions in the glass, which led to the variation of glass luminous properties. Hongli Wen et al. [9] prepared P2O5-Al2O3-SiO2-GeO2-Li2O glasses doped with 3d-transition metal ions and investigated their optical properties. Félix-Quintero et al. [10] reported the photoluminescence of Mn2+ doped zinc phosphate glasses. They all found that the change of transition metal ions coordination caused the variation in the optical and luminescence properties of glass.

As a kind of transition metal oxide, Fe2O3 has been usually added into kinds of glasses to reduce the melting temperature or used as a nucleating agent to induce nucleation and crystallization in glass-ceramics [11], [12], [13]. In the glass, iron is usually present in two valence states, i.e., Fe2+ and Fe3+. Ferrous ion (Fe2+) can be used as a network modifier to destroy the network structure of glass, while ferric ion (Fe3+) can form nets and enhance the glass networks [14, 15]. Besides, a large number of studies have also shown that Fe2O3 can significantly reduce the optical band gap of glass and promote the transition of glass from insulator to semiconductor [16], [17], [18], [19], [20]. However, we find that only a small amount of work has focused on the research of luminescence properties for Fe2O3-doped glass [21, 22]. In our previous works [23], we found that Fe2O3 can promote the formation of a single cordierite phase from the magnesium aluminosilicate-based glasses. Although the prepared glass-ceramic has a lower fluorescence lifetime, it can be used as a potential substitute material for fluorescent materials in white light-emitting diode device. Therefore, the present investigation is taken up to prepare, characterize, and study the impact of Fe2O3 content on structural and properties in MgO-Al2O3-SiO2-B2O3 (MASB) glasses, especially for the optical and fluorescence performance. We replaced Al2O3 with a small amount of Fe2O3 to prepare Fe2O3-doped MASB glasses. The glass structure, physical-chemical, optical, and luminescent properties of Fe2O3-doped MASB glasses were analyzed, and we hope that the obtained results can provide some useful guidance for the development of fluorescent materials.

Section snippets

Glass preparation

Powders of analytical reagent grade (Guo-Yao Co. Ltd., Shanghai, China), comprising magnesium oxide (MgO), aluminum oxide (Al2O3), silicon dioxide (SiO2), boric acid (H3BO3), and ferric oxide (Fe2O3), were used as the starting materials. The nominal composition of 20MgO-(20-x)Al2O3–57SiO2–3B2O3-xFe2O3 (x = 0, 0.1, 0.25, 0.5, and 1.0 mol%) were prepared by the conventional melt quenching technique, and the corresponding glass composition was named after MASB-F0, MASB-F1, MASB-F2, MASB-F3,

Analysis of XRD and DSC

Fig. 1(a) shows the prepared glasses with different Fe2O3 contents. As the Fe2O3 content increases, the color of glasses deepens gradually, i.e., from white to light yellow, yellow, and tends to tawny at last. This phenomenon is mainly caused by the colorization effect of Fe3+. Meanwhile, the transparency of the prepared glasses also decreases. Additionally, the XRD scattering spectrum of MASB glasses doped with different Fe2O3 content is also shown in Fig. 1(a). It is found that all samples

Conclusions

In the present study, a Fe2O3-doped aluminosilicate-based glass system was prepared by the traditional high-temperature melting method. The prepared glass samples are characterized by structural (DTA, XRD, FTIR), physical-chemical (density, refractive index, Vickers hardness, and acid resistance), and spectroscopic (optical absorption and photoluminescence) studies. Based on the analysis of all the studies for these glass materials, the conclusions have drawn as follows:

1) With the addition of

Data availability

The raw/processed data required to reproduce these findings cannot be shared at this time as the data also forms part of an ongoing study.

Credit author statement

Qianxing Huang: Conceptualization, Methodology, Writing-Original draft preparation.

Taoyong Liu: Investigation, Conceptualization, Resources, Data curation.

Xuefeng Shen: Software, Validation.

Xiuying Li: Investigation, Resources.

Anxian Lu: Writing-Review & Editing, Project administration, Supervision.

Yi Gu: Project administration, Supervision.

Declaration of Competing Interest

The authors declared no interest conflicts.

Acknowledgments

This work has been supported by the National Natural Science Foundation of China (no. 51672310), the Fundamental Research Funds for the Central Universities of Central South University (2019zzts934), the Natural Science Foundation of Jiangxi Province (20202BABL204020); Scientific and technological project of Jingdezhen (20192GYZD008-34).

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