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光致发光光谱能够揭示半导体材料带隙、杂质能级等电子结构信息, 还可分析界面、载流子寿命、量子效率, 在紫外-近红外波段得到广泛应用. 在约4 μm以长红外波段, 由于热背景干扰强、光致发光信号弱、探测能力低, 光致发光光谱研究长期受限. 本文介绍了利用傅里叶变换光谱仪测量光致发光光谱的常规方法, 简述了为突破红外波段困境于1989年提出、历经20多年发展的连续扫描傅里叶变换双调制光致发光光谱方法及所受机理局限; 分析了2006年报道的基于步进扫描傅里叶变换光谱仪的红外调制光致发光光谱方法的抗干扰、灵敏度、信噪比优势, 列举了国际上诸多研究组对红外调制光致发光光谱方法有效性的例证和以此取得的应用研究进展; 总结了近年来宽波段、高通量扫描成像和空间微区分辨红外调制光致发光光谱测试方法发展以及从0.56—20 μm可见-远红外宽波段覆盖到千级通道光谱高通量检测、2—3 μm微区分辨红外调制光致发光光谱技术进步, 列举了应用研究稀氮/稀铋量子阱、HgCdTe外延膜、InAs/GaSb超晶格等可见-远红外半导体材料阶段结果和合作研究典型进展. 本文展现了红外调制光致发光光谱方法先进性和宽波段、高通量扫描成像与空间微区分辨光谱测试方法有效性, 预见了未来进一步应用研究方向.
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关键词:
- 光致发光 /
- 傅里叶变换红外光谱仪 /
- 步进扫描 /
- 半导体
Photoluminescence (PL) spectroscopy has been widely used in the ultraviolet-near-infrared spectral range for over seventy years since its early reporting in the 1950’s, because it not only reveals the electronic structure information about such as band gap and impurity energy levels of semiconductor materials, but also serves as an efficient tool for analyzing interfacial structures, carrier lifetime, and quantum efficiency. However, in the infrared band beyond about 4 μm, the study of PL spectrum has been limited for decades due to strong thermal background interference, weak PL signals and low detection capability. In this review, a traditional PL method is introduced based on a Fourier transform infrared (FTIR) spectrometer, and a continuous-scan FTIR spectrometer-based double-modulation PL (csFTIR-DMPL) method is briefly described which was proposed in 1989 for breaking through the dilemma of the infrared band, and developed continuously in the later more than 20 years, with its limitations emphasized. Then, a step-scan FTIR spectrometer-based infrared modulated PL (ssFTIR-MPL) method reported in 2006 is analyzed with highlights on its advantages of anti-interference, sensitivity and signal-to-noise ratio. The effectiveness demonstration and application progress of this method in many research groups around the world are listed. Further developments in recent years are then summarized of wide-band, high-throughput scanning imaging and spatial micro-resolution infrared modulated PL spectroscopic experimental systems, and the technological progresses are demonstrated of infrared-modulated PL spectroscopy from 0.56–20 μm visible-far-infrared broadband coverage to >1000 high-throughput spectra imaging and ≤2–3 μm spatial micro-resolution. Typical achievements of collaborative research are enumerated in the visible-far-infrared semiconductor materials of dilute nitrogen/dilute bismuth quantum wells, HgCdTe epitaxial films, and InAs/GaSb superlattices. The results presented demonstrate the advancement of infrared modulated PL spectroscopy and the effectiveness of the experimental systems, and foresee further application and development in the future.
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图 1 (a) FTIR-PL光谱测试原理图. (b) 不同半导体材料PL光谱, 其中①为HgCdTe厚膜, ②为InGaNAs /GaAs量子阱(QW), ③为InGaP QW, 黑色实线为实测结果, 红色虚线是局部放大图
Fig. 1. (a) Schematic of a FTIR-PL spectroscopic system. (b) PL spectra in different spectral bands from semiconductors, where ① is the HgCdTe epilayer, ② is the InGaNAs/GaAs quantum well (QW), and ③ is the InGaP QW, black lines for measured data, red dashes for partially zoomed-in.
图 2 (a) ssFTIR-MPL光谱测试原理图[25]. (b)不同半导体材料PL光谱, 其中①为HgCdTe外延膜, ③为InGaP量子阱(QW), 黑色实线为FTIR-PL结果, 红色虚线是ssFTIR-MPL结果
Fig. 2. (a) Schematic of ssFTIR-MPL spectroscopic system[25]. (b) PL spectra in different spectral bands from semiconductors, where ① is HgCdTe epilayer, and ③ is InGaP quantum well (QW), black lines by FTIR-PL, and red dashes by ssFTIR-MPL methods.
图 3 (a) 宽波段ssFTIR-MPL光谱测试原理图; (b) InGa(N)As/GaAs量子阱(QW)低温磁光-PL光谱; (c) HgTe/HgCdTe超晶格变激发功率PL光谱; (d) 0.56—20 μm波段不同半导体PL光谱
Fig. 3. (a) Main components of wide-band ssFTIR-MPL spectroscopic experimental system; (b) low-temperature magneto-PL spectra of InGa(N)As/GaAs quantum well (QW); (c) excitation power-dependent PL spectra of HgTe/HgCdTe superlattice (SL) at 77 K; (d) PL spectra of different semiconductors in a wide spectral range of 0.56—20 μm.
图 4 (a) 扫描成像红外调制PL光谱测试原理图; (b) 532 nm泵浦光在会聚透镜和收集光抛物面反射镜公共焦点处的强度空间分布, 峰值强度1/2和$ 1/{{\mathrm{e}}}^{2} $对应光斑直径分别为15.3和26.3 μm, 插图为光斑图像[74]; (c) HgTe/HgCdTe超晶格表面5个不同坐标位置的典型 PL光谱, (720, 800)位置处PL光谱可以LE、ME和HE三个特征拟合, 插图显示实验系统使用Globar光源的响应波段范围[74]; (d)—(f) HgTe/HgCdTe超晶格样品960 μm×960 μm区域内25×25像素PL光谱LE, ME和HE拟合特征的能量、强度和FWHM图像[74]
Fig. 4. (a) Main components of scanning imaging IR-MPL spectroscopic system; (b) spatial profile of 532 nm pumping light intensity at the common focal point of the lens and parabolic mirror, 1/2 and $ 1/{{\mathrm{e}}}^{2} $ peak intensities correspond to spot diameters of 15.3 and 26.3 μm, respectively, insert for spot picture[74]; (c) typical PL spectra of HgTe/HgCdTe superlattice at 5 different coordinate positions, that at (720, 800) fitted with LE, ME and HE PL features, inset for system response with inner globar source[74]; (d)–(f) energy, intensity, and FWHM images of the LE, ME, and HE PL features of 25×25-pixel PL spectra on a 960 μm×960 μm surface part of HgTe/HgCdTe superlattice[74].
图 5 (a) IRM-μPL光谱测试原理图; (b) 激光定位在InAs/GaSb 超晶格不同台面和凹槽上的代表性μPL光谱, 竖直虚线显示低能PL光谱分量峰值能量变化, 插图所示样品μPL测试区域的表面光学形态[78]; (c) InAs/GaSb 超晶格测试区低能PL光谱分量积分强度微区空间分布[78]
Fig. 5. (a) Main components of the IRM-μPL spectroscopic system; (b) representative μPL spectra recorded at different mesas and grooves, low- and high-energy PL components from infrared absorption layer and electron barrier layer of InAs/GaSb superlattice, vertical dashes for peak energy variation of the low-energy PL component, inset for optical morphology of the μPL mapped area[78]; (c) spatial distribution of integral intensity of the low-energy PL component in the measured area of InAs/GaSb superlattice[78].
表 1 不同研究组(报道)扫描成像红外PL光谱空间分辨率等参数比较
Table 1. Comparison of spatial resolution and other parameters of scanning imaging infrared PL spectroscopy by different research groups.
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