Research Progress of Materials and Detectors for Mid-wave Infrared Quantum Dots
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摘要: 量子点（Quantum dots，QDs）由于本身所具有的量子限域效应、尺寸效应和表面效应等各种特性，被广泛应用于光电探测、生物医学、新能源等方面。而中波红外（Mid-wave infrared，MWIR）量子点作为近年来红外领域的研究热点，通过调整控制其尺寸的大小，能够扩展其红外吸收波长。因此，成功制备中波红外量子点材料和器件对红外成像、红外制导和搜索跟踪等方面有着重要意义。本文首先介绍了HgSe、HgTe、PbSe、Ag2Se和HgCdTe五种中波红外量子点材料制备合成技术，分析了量子点的尺寸形貌、晶格条纹以及红外吸收光谱等特性，然后对国内外中波红外量子点探测器进行了归纳总结，概述了探测器的器件结构、制备方法，并对器件的响应率、探测率以及响应时间等光电性能参数进行了对比分析。最后，对中波红外量子点的发展进行了展望。Abstract: Quantum dots (QDs) are widely used in photoelectric detection, biomedicine, new energy, and other fields because of their quantum limitations, size, and surface effects. Recent years have seen midwave infrared (MWIR) quantum dots (QDs) become a focal point in infrared research. By adjusting and controlling their size, these QDs can extend their absorption wavelengths in the infrared spectrum. Therefore, the successful preparation of infrared QD materials and devices is crucial for infrared imaging, guidance, search, and tracking. This study first introduces the preparation and synthesis technology of five types of MWIR QDs materials, HgSe, HgTe, PbSe, Ag2Se, and HgCdTe, analyzes the size and morphology, lattice fringe, and infrared absorption spectrum characteristics of the QDs, and then summarizes the domestic and foreign MWIR QDs detectors. The device structures and preparation methods of the detector are summarized, and the photoelectric performance parameters, such as responsivity, detectivity, and response time, of the detectors are compared and analyzed. Finally, the development of MWIR QDs was discussed.
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Key words:
- quantum dots /
- mid-wave infrared /
- photodetector
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图 2 HgSe CQDs的形貌结构、PL光谱及其吸收光谱：HgSe CQDs的(a) TEM图像；(b) 不同反应时间的吸收光谱以及(c) PL光谱[26]；HgSe CQD的(d)15.5 nm粒径TEM图像和(e)不同尺寸的吸收光谱[20]；(f)HgSe CQDs的TEM图像[24]；(g)HgSe CQDs的TEM图像和(h)吸收光谱[25]；(i)不同合成条件下的HgSe和HgTe CQDs的吸收光谱[23]
Figure 2. Morphology structures, PL spectra and absorption spectrum of HgSe CQDs: (a) TEM image, (b) Absorption spectrum with different reaction times and (c) PL spectra of HgSe CQDs[26]; (d) 15.5 nm particle size TEM image and (e) Absorption spectrum with different particle sizes of HgSe CQDs[20]; (f) TEM image of HgSe CQDs[24]; (g) TEM image and (h) Absorption spectrum of HgSe CQDs[25]; (i) Absorption spectra of HgSe and HgTe CQDs with different synthesis conditions[23]
图 3 HgTe、PbSe和Ag2Se CQDs的形貌结构、粒径分布及其吸收光谱：(a)HgTe Ncs的TEM图像和吸收光谱[47]；HgTe CQDs的(b)TEM图像和(c)吸收光谱[19]；(d)不同尺寸HgTe CQDs的吸收光谱[21]；HgTe CQDs的(e)TEM图像，插图为HRTEM图像和(f)粒径分布[18]；PbSe CQDs的(g)TEM图像及其(h)粒径分布[32]；(i)Ag2Se CQDs的粒径分布[35]
Figure 3. Morphology structures, particle size distributions and absorption spectra of HgTe, PbSe and Ag2Se CQDs: (a) TEM images and absorption spectrum of HgTe Ncs[47]; (b) TEM image and (c) Absorption spectrum of HgTe CQDs[19]; (d) Absorption spectrum of HgTe CQDs with different sizes[21]; (e) TEM image, insert is HRTEM image and (f) Particle size distribution of HgTe CQDs[18]; (g) TEM image and (h) Particle size distribution of PbSe CQDs[32]; (i) Particle size distribution of Ag2Se CQDs[35]
图 4 Ag2Se和HgCdTe CQDs的形貌结构及其吸收光谱：Ag2Se CQDs的(a)TEM图像与(b)吸收光谱[36]；(c)7.3 nm的Ag2Se CQDs的TEM图像，插图为选区电子衍射图[35]；(d)不同粒径尺寸Ag2Se CQDs薄膜的FTIR吸收光谱[35]；HgCdTe CQD的(e)TEM图像和(f)吸收光谱[30]；HgCdTe CQD的(g)TEM图像；(h)HRTEM图像和(i)吸收光谱[29]
Figure 4. Morphology structures and absorption spectrum of Ag2Se and HgCdTe CQDs: (a) TEM images and (b) Absorption spectrum of Ag2Se CQDs[36]; (c) TEM image of 7.3 nm Ag2Se CQDs, insert is a selection electron diffraction pattern[35]; (d) FTIR absorption spectrum of Ag2Se CQDs films with different particle sizes[35]; (e) TEM image and (f) Absorption spectrum of HgCdTe CQDs[30]; (g) TEM image, (h) HRTEM image and (i) absorption spectrum of HgCdTe CQDs[29]
图 5 HgTe CQDs和SMLQD-QCD中波红外探测器的性能：(a)量子级联和表面等离子体耦合结构的中波红外反射和增强光谱[50]；(b)HgTe CQDs的首次中波红外成像图[52]；四色HgTe CQDs探测器的(c)探测率曲线和(d)响应率曲线[16]；SMLQD-QCD的(e)器件结构图；(f)响应率曲线；(g)不同温度的暗电流曲线以及(h)探测率曲线[61]；(i)单层量子点p-i-n器件的响应率曲线[64]
Figure 5. Performances of MWIR detector for HgTe CQDs and SMLQD-QCD: (a) MWIR reflection and enhancement spectrum of QCD and surface plasmon coupled structure[50]; (b) First MWIR imaging of HgTe CQDs[52]; (c) Detectivity curve and (d) Responsivity curves of four-color HgTe CQDs detector[16]; (e) Structure diagram, (f) Responsivity curves, (g) Dark current curves with different temperatures, and (h) Detectivity curves of MLQD-QCD[61]; (i) Responsivity curves of single layer quantum dot p-i-n device[64]
图 6 HgTe CQDs和PbSe CQDs中波红外探测器的性能测试：不同截止波长HgTe CQDs器件随温度变化的响应率曲线(a)样品A为2.8 μm；(b)样品B为3.4 μm，(c)样品C为5.3 μm以及(d)样品C的暗电流曲线，插图为70 K和210 K下的I-V曲线[18]；(e)HgTe CQDs中波红外探测器5 V偏压下的探测率[10]；4.8 μm像元的HgTe CQDs器件不同偏压下的(f)响应率曲线和(g)探测率曲线[21]；(h)不同尺寸HgTe CQDs薄膜的吸收光谱[20]；(i)PbSe CQDs上转换中波红外光电探测器的响应率曲线[65]
Figure 6. Performances testing of HgTe CQDs and PbSe CQDs MWIR detector: Responsivity curves of different cut-off wavelength HgTe CQDs device with changed temperatures (a) Sample A 2.8 μm, (b) Sample B 3.4 μm, (c) Sample C 5.3 μm and (d) Dark current curves of sample C, insert is the I-V curves at 70 K and 210 K[18]; (e) Detectivity of HgTe CQD MWIR detector at 5 V bias[10]; (f) Responsivity curves and (g) Detectivity curves of 4.8 μm pixel HgTe CQDs device at different bias voltage[21]; (h) Absorption spectra of HgTe CQDs films with different size[20]; (i) Responsivity curves of PbSe CQDs up-conversion mid-wave infrared photodetector[65]
图 7 HgTe CQDs中波红外探测器的器件结构及其性能：HgTe CQDs器件的(a)结构图和不同温度下的(b)光电流曲线，(c)响应率曲线，(d)探测率曲线和(e)暗电流曲线[56]；HgTe CQDs光导器件的(f)响应率曲线和(g)探测率曲线[54]；等离激元增强HgTe CQDs探测器的(h)器件结构和(i)响应率曲线[58]
Figure 7. Device structures and performances of HgTe CQDs MWIR detectors: (a) Structure diagram and (b) Photocurrent curves, (c) Responsivity curves, (d) Detectivity curves and (e) Dark current curves of HgTe CQDs device with different temperatures[56]; (f) Responsivity curves and (g) Detectivity curves of HgTe CQDs photoconductive device[54]; (h) Device structure and (i) Responsivity curve of plasmon enhanced HgTe CQDs detector[58]
图 8 HgTe、HgSe CQDs中波红外探测器的器件结构、性能及焦平面成像：(a)SWIR/MWIR双波段HgTe CQDs探测器的器件结构[53]；不同偏压下4.2 μm HgSe CQDs器件的(b)光电流曲线和(c)响应率曲线[25]；(d)SWIR/MWIR双波段HgTe CQDs探测器在不同温度下的探测率曲线[53]；(e)9 V偏压下4个不同波长的HgSe CQDs器件的响应率曲线[25]；(f)具有纳米片结构的4.2 μm HgSe CQDs探测器的响应率曲线[25]；HgTe/HgSe CQDs复合光电二极管的(g)器件结构和(h)I-V曲线[23]；(i)640×512 HgTe CQDs中波红外焦平面热成像[67]
Figure 8. Device structures, performances, and FPA imaging of HgTe and HgSe CQDs MWIR detectors: (a) Device structure of SWIR/MWIR dual-band HgTe CQDs detector[53]; (b) Photocurrent curves and (c) Responsivity curves of 4.2 μm HgSe CQDs devices[25]; (d) Detectivity curves of SWIR/MWIR dual-band HgTe CQDs detector under different bias voltages[53]; (e) Responsivity curves of four devices with different wavelength at 9 V bias voltage[25]; (f) Responsivity curves of 4.2 μm HgSe CQDs detector with nano-disks[25]; (g) Device structure and (h) I-V curves of HgTe/HgSe CQDs mixed photodiode[23]; (i) 640×512 HgTe CQDs MWIR FPA thermal imaging[67]
表 1 不同中波红外量子点材料及其主要性能指标
Table 1. Different MWIR quantum dot materials and their main performance merits
Quantum dot materials Preparation method Grain size/nm Absorption wavelength/µm Ref. Quantum dot materials Preparation method Grain size/nm Absorption wavelength/µm Ref. HgTe Water-based synthetic 3-12 1.2-3.7 [13] HgCdTe Hot injection 8-11 2.2-5 [28] Two-step injection 14.5 1.3-5 [14] ~14 3 [29] Colloidal atomic layer deposition (c-ALD) 9-10 5 [15] Chemical synthesis 15-16 2-7 [30] Hot injection 10-16 2-5 [16] PbSe Chemical synthesis 10-17 4.1 [31] 5-15 2.2-3.3 [17] Hot injection ~18 3.3-3.5 [32] 6-12 2.8-7 [18] 30 2.5-5 [33] 5-15 1.5-5 [19] 20-100 1-25 [34] ~15 3-5 [20] Ag2Se Hot injection 7.3 5.6 [35] ~20 2-10 [21] 5-6 2-5 [36] HgSe - 10 3-20 [22] 5-28 4.8 [37] Hot injection 4-6 2-5 [23] - 4.1 [38] 4.7 3.3-5 [24] - 5 [39] 10-15 3-10 [25] 8-10 3-5 [40] 6.2 3-5 [26] 5 4.2 [41] 5.4 4.2 [27] 5.5 4.2 [42] 
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表 2 中波红外量子点探测器件的量子点薄膜的制备方法、器件结构及其主要性能参数[53-63]
Table 2. Preparation method, device structure and main performance parameters of quantum dot film for MWIR quantum dot detector[53-63]
Preparation method of QD thin film Device structure Response wavelength/µm R/(A/W) D*/Jones Response time/µs Ref. Spray-coating HgTe QDs/Au/Cr/PET 2-5 0.9 8×109 - [16] Spin-coating QDs/Au/Si/SiO2 ~7 - 107-109 0.2 [17] Au/HgSe-HgTe/Al/Sapphire 4.4 - 1.5×109 < 0.5 [26] Pt/HgTe CQDs/HgSe 4.2 1.45×10-3 - - [25] Au/HgCdTe CQDs/p-Si/Al 3.5 - 1.6×108 - [30] Ag/Ag2Se QDs/PbS QD/Ag2Se QDs/Ag/Cr/Sapphire 4.2 13.3 3×105 - [41] Al/ZnO/ Ag2Se CQDs-PbS CQDs/MoOx/Au/Cr/Glass 4.2 19 7.8×106 - [42] Au/Bi2Se3/HgTe CQDs/Ag2Te/HgTe CQDs/Bi2Se3/ITO/Al2O3 3-5 - 3×1010 - [53] PMMA/HgTe CQDs/SiO2/Si 5 0.23 5.4×1010 2.9 [54] Drop-casting Pt/HgTe CQDs/Pt/Glass 2.8-7 > 0.1 2×109 < 0.1 [18] Pt/HgTe CQDs/Pt 1.5-5 ≈1×10-3 1010 - [19] Pt/HgSe CQDs/Pt/ZnSe 2.5-5 5×10-4 8.5×108 - [26] Ag2Se CQDs/ZnO/Al2O3/Glass 2-5 - - - [36] Au/Ag2Se CQDs/SiO2/Si 4.1 0.35 - - [33] HgCdTe CQD/Au/Sapphire 2.5-5 8.9×10-4 108 - [55] HgTe CQDs/Si 3-5 0.15-0.25 2×109 - [10] Au/Ag2Te CQDs/HgTe CQDs/ ITO/Al2O3 3.8-4.8 0.38 1.2×1011 1.3 [56] Pt/HgTe CQDs/Pt 3.5 0.1 3.5×1010 - [57] Layer-by-layer deposition Pd/HgTe CQDs/Ti/SiO2/Si ~6.5 1.8×10-3 1.3×109 < 5 [20] HgTe CQDs/PMMA/Si/SiO2 2-10 ~0.1 2×107 - [21] Au/Ag2Se QDs/SiO2/Si 4.8 8×10-3 - - [37] Au/Ag2Se CQDs/SiO2/Si 5 1.66 - - [39] HgTe CQDs/ROIC/LCC 3.6 - 2×1010 - [51] Au/SiO2/Au+ITO/HgTe QDs/Plasmonic nano-disks/ITO/Al2O3 ~4.5 1.62 4×1011 - [58] PbS QDs/Au/CaF2 5-9 1.5×10-4 4×104 - [59] MBE P3-P2-P1-Hg1-xCdxTe 2.5-5.1 - 2.02×1011 - [60] n-GaAs/SML-QDS/DFLS/n-GaAs/Si 5-8 5.9×10-4 3×1010 - [61] Au/Ti/In0.53Ga0.47As/In0.52Al0.48As/Au/Ti/InP 5.8-10.4 6×10-4 2.6×108 - [62] Dip-coating Ag/HgTe CQDs/NiCr/CaF2 2.2-6.7 > 0.38 > 1010 - [63]
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