Pine-shaped AlN:Er<sup>3+</sup> nanostructure: A multifunctional material with both luminescent and magnetic properties

DING Xin; TIAN Zifeng; WANG Qiushi; LIU Cailong; CUI Hang

doi:10.7498/aps.74.20241587

Abstract

Erbium-doped aluminum nitride (AlN:Er³⁺) pine-shaped nanostructures are synthesized, through a direct reaction between aluminum (Al) and erbium oxide (Er₂O₃) mixed powders in a nitrogen (N₂) atmosphere, by using a direct current arc discharge plasma method. X-ray diffraction (XRD) analysis reveals that the diffraction peaks of AlN:Er³⁺ shift towards lower angles for the doped sample compared with those of undoped AlN, indicating lattice expansion due to Er³⁺ incorporation. X-ray photoelectron spectroscopy (XPS) confirms that Al, N, and Er are coexistent, while energy-dispersive X-ray spectroscopy (EDS) quantitatively shows that the atomic ratio for Al:N:Er is about 46.9∶52.8∶0.3. The nanostructures, resembling pine trees, are measured to be 5–10 μm in height and 1–3 μm in width, with branch nanowires extending 500 nm–1 μm in length and 50–100 nm in diameter. These branches, radiating at about 60° from the main trunk, are found to grow along the [100] direction of wurtzite-structured AlN, as evidenced by high-resolution transmission electron microscopy (HRTEM) showing lattice spacing of 0.27 nm corresponding to the (100) plane. Photoluminescence studies identify distinct emission peaks in the visible region (527, 548, and 679 nm) and near-infrared region (801, 871, and 977 nm), which is attributed to intra-4f electron transitions of Er³⁺ ions. The average lifetime of the excited state at 548 nm is measured to be 9.63 μs, slightly shorter than those of other Er³⁺-doped materials. The nanostructures demonstrate that the superior temperature sensing capability possesses a maximum relative sensitivity of 1.9×10^–2 K^–1 at 293 K, based on the fluorescence intensity ratio of thermal-coupled levels (²H_11/2/⁴S_3/2). Magnetic characterization reveals that the room-temperature ferromagnetism has a saturation magnetization of 0.055 emu/g and a coercive field of 49 Oe, with a Curie temperature exceeding 300 K, which shows the potential for room-temperature spintronic applications. First-principle calculations attribute the observed ferromagnetism to Al vacancies, whose formation energy is significantly reduced by Er doping, leading to a high concentration of Al vacancies. These findings highlight the potential of AlN:Er³⁺ pine-shaped nanostructures in various applications, including optoelectronics, temperature sensing, and dilute magnetic semiconductors.

Keywords:

Authors and contacts

1.
College of Physical Science and Technology, Bohai University, Jinzhou 121013, China
2.
College of Physical Science and Information Engineering, Liaocheng University, Liaocheng 252000, China
3.
College of Physics, Jilin University, Changchun 130000, China

Corresponding author: WANG Qiushi, wang_jiu_jiu@foxmail.com

Funds: Project supported by the National Key Research and Development Program of China (Grant No. 2023YFA1406200) and the National Natural Science Foundation of China (Grant No. 11874174).

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References

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Cited By

图 1 未掺杂AlN和AlN:Er³⁺松树状纳米结构的XRD图谱(插图为(100), (002), (101)峰的放大图)

Figure 1. XRD patterns of undoped AlN and AlN:Er³⁺ pine-shaped nanostructure (the enlarged (100), (002) and (101) peaks in inset).

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图 2 AlN:Er³⁺松树状纳米结构的(a) XPS全图谱, 以及(b) Al 2p, (c) N 1s, (d) Er 4d的高分辨率图谱

Figure 2. XPS patterns of AlN:Er³⁺ pine-shaped nanostructure: (a) Survey spectrum; high resolution spectra for (b) Al 2p, (c) N 1s, (d) Er 4d.

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图 3 (a)—(c) AlN:Er³⁺松树状纳米结构从低倍到高倍的SEM图像; (d) EDS图谱

Figure 3. (a)–(c) Scanning electron microscopy images from low to high magnification of AlN:Er³⁺ pine-shaped nanostructure; (d) EDS spectrum.

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图 4 AlN:Er³⁺松树状纳米结构的(a) TEM图像、(b) HRTEM图像、(c) FFT图像和(d) EDS元素映射图像

Figure 4. (a) TEM image, (b) HRTEM image, (c) FFT pattern and (d) EDS element mapping of AlN:Er³⁺ pine-shaped nanostructure.

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图 5 (a)未掺杂的AlN和AlN:Er³⁺松树状纳米结构的漫反射光谱; (b) AlN:Er³⁺松树状纳米结构在548 nm处的激发光谱; (c)室温下AlN:Er³⁺松树状纳米结构在可见光(378 nm激发)到红外光(532 nm激发)范围内的发射光谱(插图为可见光范围内的光致发光成像); (d) Er³⁺能级跃迁图

Figure 5. (a) DRSs of undoped AlN and AlN:Er³⁺ pine-shaped nanostructure; (b) excitation spectrum of AlN:Er³⁺ pine-shaped nanostructure at 548 nm; (c) the room-temperature Vis-NIR emission spectrum of AlN:Er³⁺ pine-shaped nanostructure (the visible PL imaging in inset); (d) the schematic energy level diagram for Er³⁺ ions.

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图 6 548 nm处的PL衰减曲线

Figure 6. PL decay curve at 548 nm.

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图 7 (a)不同温度下AlN:Er³⁺松树状纳米结构的PL光谱; (b) AlN:Er³⁺松树状纳米结构在293—553 K的FIR (I_{527 nm}/I_{548 nm})及对其随温度变化线性拟合结果(三角形标记代表FIR的实验值, 虚线为拟合曲线); 相对灵敏度S_r随温度的变化(菱形标记代表S_r的值)

Figure 7. (a) Temperature-dependence spectra of AlN:Er³⁺ pine-shaped nanostructure; (b) FIR values of AlN:Er³⁺ pine-shaped nanostructure at the temperature of 293−553 K and the linear fitted results between the FIR and the temperature (the triangular markers represent the experimental values of FIR, and the dashed line is the fitting curve); the variation of relative sensitivity (S_r) with temperature (the diamond markers represent the values of S_r).

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图 8 (a)室温下AlN:Er³⁺松树状纳米结构的磁滞回线; (b)单位磁化强度随温度的变化

Figure 8. (a) Magnetization hysteresis loops of AlN:Er³⁺ pine-shaped nanostructure measured at room temperature; (b) variation of unit magnetization intensity with temperature.

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图 9 自旋极化态密度图　(a) Er_Al体系; (b) Er_Al + V_N体系; (c) Er_Al + V_Al体系; 正值为自旋向上, 负值为自旋向下, 费米能级用垂直虚线来表示

Figure 9. Total DOS and partial DOS of Er atom, Al atom and N atom for (a) Er_Al system, (b) Er_Al + V_N system, (c) Er_Al + V_Al system. The Fermi level is indicated by the vertical dashed line.

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图 10 自旋电荷密度的空间分布　(a) Er_Al体系; (b) Er_Al + V_N体系; (c) Er_Al + V_Al体系

Figure 10. Spatial distribution of the spin density: (a) Er_Al system; (b) Er_Al + V_N system; (c) Er_Al + V_Al system.

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表 1 基于FIR技术对Er³⁺掺杂不同材料的相对灵敏度(S_r)进行比较

Table 1. Comparison of relative sensitivity (S_r) of Er³⁺ doped different materials based on FIR technology.

Er³⁺掺杂不同材料	S_r范围/(10^–2 K^–1)	T范围/K	文献	年份
AlN松树状纳米结构	0.53—1.9	293—553	本文	2024
AlN薄膜	0.25—2.2	110—550	[34]	2023
Sr₉Y₂W₄O₂₄	~1.33	293—443	[48]	2024
La₂MgTiO₆	~1.12	303—483	[54]	2021
LaGdO₃	0.1—1.2	298—900	[55]	2019
Ag@NaGdF₄	~0.42	298—573	[56]	2019
Sr₂YbF₇	~0.62	300—500	[57]	2015

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表 2 V_Al和Er_Al + V_Al体系在富Al和富N条件下的形成能

Table 2. Formation energy under the Al-rich and N-rich conditions of the V_Al and Er_Al + V_Al systems.

体系	形成能/eV
体系	富Al	富N
V_Al	9.1935	6.1735
Er_Al + V_Al	10.35831	4.31831

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[15]	Rougab M, Gueddouh A 2021 Appl. Phys. A 127 969 Google Scholar
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Pine-shaped AlN:Er³⁺ nanostructure: A multifunctional material with both luminescent and magnetic properties

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Pine-shaped AlN:Er3+ nanostructure: A multifunctional material with both luminescent and magnetic properties

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Pine-shaped AlN:Er³⁺ nanostructure: A multifunctional material with both luminescent and magnetic properties