Electrical and magnetic properties of (In, Co) co-doped ZnO films deposited using radio frequency magnetron sputtering
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摘要: (In, Co)共摻的ZnO薄膜（ICZO薄膜）在100 ℃下通過射頻（RF）濺射沉積至玻璃基板上。沉積過程采用In、Co、Zn三靶共濺射。通過調節靶功率，獲得了不同In含量的ICZO薄膜。研究了不同In含量下薄膜電學性質和磁學性質的變化。分別使用掃描電子顯微鏡（SEM）、高分辨透射電子顯微鏡（HR-TEM）、原子力顯微鏡（AFM）、電子探針掃描（EPMA）、X射線衍射儀(XRD)、霍爾測試（Hall measurement）和振動樣品磁強計（VSM）對薄膜的成分、形貌、結構、電學特性和磁學特性進行了表征和分析。詳細分析了薄膜中載流子濃度對磁學性質的影響。實驗結果表明，隨著薄膜中In含量的提高，薄膜中載流子濃度顯著提高，薄膜的導電性得到優化。所有的薄膜均表現出室溫下的鐵磁特性。與此同時，束縛磁極化子（BMP）模型與交換耦合效應兩種不同的機制作用于ICZO半導體材料，致使薄膜的飽和磁化強度隨載流子濃度發生改變，并呈現在三個不同的區域。Abstract: Diluted magnetic semiconductors (DMSs) have attracted much attention in recent years due to their dual control of charge and spin degrees of freedom in carriers. Potential applications of DMSs include spin light-emitting diodes, spin field-effect transistors, magnetoresistance random access memory, and ultrafast optical switches. However, the Curie temperature (Tc) of most DMSs below ambient temperature limits the efficiency of these devices. Thus, the biggest challenge for developing DMS materials has been producing host materials that exhibit ferromagnetic behavior above ambient temperature. A series of theoretical simulations and experiments show that the Tc value of ZnO-based DMSs could satisfy this requirement. Incorporation of selective transition metal elements (e.g., Fe2+, Co2+, Ni2+, and Mn2+) has been confirmed as an effective way to enhance the magnetic properties of ZnO. In the present research, (In, Co) co-doped ZnO (ICZO) films were deposited by radio frequency sputtering at 100 ℃ on a glass substrate. The sputtering process was performed through In, Co, and ZnO co-sputtering. The presence of ICZO films has been adjusted by changing the target sputtering power. The variation of electric and magnetic properties of the film was studied with different In content. The composition, morphology, structure, electric and magnetic properties of films were characterized by field emission scanning electron microscopy, high-resolution transmission electron microscopy, atomic force microscopy, electron probe microanalyzer, X-ray diffractometer, Hall effect analysis, and vibrating sample magnetometer. The effect of carrier concentration on the magnetic properties of the film was analyzed extensively. These results show that, in the presence of In, the carrier concentration increases, thereby optimizing films’ conductivity. All the films present ferromagnetic behavior at room temperature. Besides, with an influence of bound magnetic polaron model and carrier-mediated exchange mechanisms on the film’s saturation magnetization, carrier-concentration dependent behavior can be expressed in three different regions.
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圖 1 (In, Co)?ZnO薄膜中In含量隨著In2O3靶功率的變化
Figure 1. In content in (In, Co)?ZnO thin films as a function of the sputtering power applied on In2O3 target
圖 2 不同In含量的(In, Co)-ZnO薄膜的X射線衍射圖
Figure 2. X-ray diffraction patterns of (In, Co)-ZnO films with various In2O3 contents
圖 3 薄膜的表面掃描電鏡圖像和原子力顯微鏡圖像。（a） 純ZnO；（b）（In, Co）?ZnO（In原子數分數3.4%)
Figure 3. Top surface SEM micrographs and AFM images: (a) pure ZnO; (b) (In, Co)?ZnO (atomic ratio of In is 3.4%)
圖 4 薄膜的橫截面透射電鏡圖像。（a）純ZnO;（b）（In, Co）?ZnO（In原子數分數3.4%）；（a1）圖（a）紅色區域放大圖；（b1）圖（b）紅色區域放大圖
Figure 4. Cross-sectional TEM images: (a) pure ZnO; (b) (In Co)?ZnO (atomic ratio of In is 3.4%); (a1) the magnified images from the portions marked with red dotted squares of Fig.4(a); (b1) the magnified images from the portions marked with red dotted squares of Fig.4(b)
圖 5 (In, Co)?ZnO薄膜電學性質隨In原子數分數的變化。（a）載流子遷移率與載流子濃度的變化；（b）薄膜導電率的變化
Figure 5. Electrical properties of (In, Co)?ZnO films with various In contents: (a) the variation of the carrier mobility and carrier concentration; (b) the variation of the film’s conductivity
圖 6 (In, Co)?ZnO薄膜磁化強度隨In原子數分數的變化
Figure 6. Magnetic properties of (In, Co)?ZnO films with various In atomic ratio
圖 7 (In, Co)?ZnO薄膜飽和磁化強度（Ms）與載流子含量的關系
Figure 7. Relationship between saturation magnetization (Ms) and carrier concentration of (In, Co)?ZnO films
表 1 Co?ZnO和(In, Co)?ZnO薄膜的沉積參數
Table 1. Sputtering parameters maintained during the deposition of Co-ZnO and (In, Co)-ZnO thin films
Background
pressure/PaWorking
pressure/PaWorking
gasHot
substrate/KFilm
thickness/nmSubstrate Draw
distance/cmSputtering
power/WZnO Co In2O3 < 6.7 × 10?4 1.67 Ar 373 100 Glass 10 80 15→10 0→25 
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