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Quantum cascade technology, based on resonant tunneling and intersubband transitions in a multiple-quantum well or superlattice structure can generate light source and detect optical signals, it is the theoretical cornerstone of quantum cascade laser(QCL) and quantum cascade detector (QCD), which has wide application prospect in detection, remote sensing, communication, ra-dar, and other fields. After three decades of research, quantum cascade technology has made significant progress in basic research,product performance, application system research and scene testing. In this paper, the principle and development history of quantum cascade technology are briefly introduced first. Subsequently, the calculation approaches of intersubband energy level structure and electron transport dynamics in quantum cascade devices are elaborated. Next, the research progress of quantum cascade technology is mainly reviewed, including mid- and far-infrared high power QCL, mid-and far-infrared widely tunable QCL, terahertz QCL, high performance QCD, and single-chip photonic integration of QCL and QCD. Finally, the commercially available QCL and QCD products, as well as their application status, are introduced.

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量子级联技术基于多量子阱或超晶格结构中的子带跃迁和共振隧穿理论,既可以产生光源,又可以探测光信号,是量子级联激光器(QCL)和量子级联探测器(QCD)的理论基石,在检测、遥感、通信、雷达等领域具有广泛的应用前景。经过最近三十年的研究,量子级联技术在基础研究、产品性能以及应用系统研发和场景试验方面都取得了重大进展。本文首先简要介绍了量子级联技术的原理和发展历史,随后阐述了量子级联器件子带能级结构和电子输运动力学计算思路,接着重点综述了量子级联技术的研究进展,包括中远红外高功率QCL、中远红外宽调谐QCL、太赫兹QCL、高性能QCD,以及QCL和QCD的单芯片光子集成方面的内容,最后介绍了QCL和QCD的产品与应用情况。

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杨超 1988年生,博士,工程师。

李泰澎 2000年生,硕士研究生。

黄宝玉 1992年生,讲师,硕士生导师。

李愽乐 2001年生,硕士研究生。

张盛楠 1994年生,博士后,工程师。

黄彦 1990年生,博士,高级工程师。

王兆刚 1990年生,博士,高级工程师。

史青 1982年生,博士,研究员。

尹玉刚 1982年生,硕士,研究员。

彭泳卿 1980年生,博士,研究员。

李晓干 1976年生,教授,博士生导师。

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Boston, MA, USA: Massachusetts Insti-tute of Technology, 2020., articleTitle=New frontiers in THz quantum cas-cade lasers, refAbstract=null), Reference(id=1241113421727453533, tenantId=1146029695717560320, journalId=1238841944844054536, articleId=1241110430186262891, doi=null, pmid=null, pmcid=null, year=2018, volume=null, issue=null, pageStart=null, pageEnd=null, url=null, language=null, rfNumber=[130], rfOrder=149, authorNames=SILVA J G, MIRZAEI B, LAAUWEN W, journalName=null, refType=null, unstructuredReference=SILVA J G, MIRZAEI B, LAAUWEN W, et al. 4×2 HEB receiver at 4.7 THz for GUSTO[C]//Millimeter, Submillimeter, and Far-Infrared Detectors and Instru-mentation for Astronomy IX, 2018., articleTitle=4×2 HEB receiver at 4.7 THz for GUSTO, refAbstract=null), Reference(id=1241113421781979486, tenantId=1146029695717560320, journalId=1238841944844054536, articleId=1241110430186262891, doi=null, pmid=null, pmcid=null, year=null, volume=null, issue=null, pageStart=null, pageEnd=null, 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Research progress in performances of responsivity and detectivity of quantum cascade detector

, figureFileSmall=null, figureFileBig=null, tableContent=
Detection wavelength/μmResponsivity/(mA/W)Detectivity/(cm·Hz1/2·W-1)Operating temperature/KResearch institutionsYearReferences
4.60.121.63×106150University of Neuchâtel2002[97]
848.65×10710University of Neuchâtel, etc2004[98]
9.2357×10950Thales Research and Technology, etc2004[16]
10.58~10>×10950University of Neuchâtel, etc.2009[59]
4.78~91×101150University of Neuchâtel, etc.2009[59]
4.18.4~109160Institute of Semiconductors, Chinese Academy of Sciences2012[99]
816.8~107300Vienna University of Technology, etc2014[100]
4.8, 5.8403.1×101080Princeton University, etc.2015[101]
4.841.92.7×107300Vienna University of Technology2015[102]
4.3165×107300Vienna University of Technology, etc.2016[103]
5.472.5×107300Hamamatsu Photonics2016, 2017[104]
5.4403.5×107300Hamamatsu Photonics2016, 2017[104]
4.113007×107300Vienna University of Technology2017[40]
7.6~10.4635.1×10977Shanghai Institute of Technical Physics, Chinese Academy of Sciences2019[105]
950107~108300University of Paris, etc.2020[106]
8.65.24.18×106300Institute of Semiconductors, Chinese Academy of Sciences, etc2021[11]
104.15/290Institute of Semiconductors, Chinese Academy of Sciences, etc2021[11]
182.34101115Institute of Semiconductors, Chinese Academy of Sciences, etc2021[11]
2.75.631.14×108293Vienna University of Technology, etc.2022[107]
10.385/295French Joint Laboratory of III-V Lab, etc.2022[21]
4.6156.91.9×101180Tsinghua University, etc.2023[108]
13~161.451.52×101215Fudan University, etc.2023[109]
14.53.511×10877Changchun University of Science and Technology, etc2023[110]
), ArticleFig(id=1241113405440970948, tenantId=1146029695717560320, journalId=1238841944844054536, articleId=1241110430186262891, language=CN, label=表1, caption=

量子级联探测器在响应率和探测率性能方面的研究进展

, figureFileSmall=null, figureFileBig=null, tableContent=
Detection wavelength/μmResponsivity/(mA/W)Detectivity/(cm·Hz1/2·W-1)Operating temperature/KResearch institutionsYearReferences
4.60.121.63×106150University of Neuchâtel2002[97]
848.65×10710University of Neuchâtel, etc2004[98]
9.2357×10950Thales Research and Technology, etc2004[16]
10.58~10>×10950University of Neuchâtel, etc.2009[59]
4.78~91×101150University of Neuchâtel, etc.2009[59]
4.18.4~109160Institute of Semiconductors, Chinese Academy of Sciences2012[99]
816.8~107300Vienna University of Technology, etc2014[100]
4.8, 5.8403.1×101080Princeton University, etc.2015[101]
4.841.92.7×107300Vienna University of Technology2015[102]
4.3165×107300Vienna University of Technology, etc.2016[103]
5.472.5×107300Hamamatsu Photonics2016, 2017[104]
5.4403.5×107300Hamamatsu Photonics2016, 2017[104]
4.113007×107300Vienna University of Technology2017[40]
7.6~10.4635.1×10977Shanghai Institute of Technical Physics, Chinese Academy of Sciences2019[105]
950107~108300University of Paris, etc.2020[106]
8.65.24.18×106300Institute of Semiconductors, Chinese Academy of Sciences, etc2021[11]
104.15/290Institute of Semiconductors, Chinese Academy of Sciences, etc2021[11]
182.34101115Institute of Semiconductors, Chinese Academy of Sciences, etc2021[11]
2.75.631.14×108293Vienna University of Technology, etc.2022[107]
10.385/295French Joint Laboratory of III-V Lab, etc.2022[21]
4.6156.91.9×101180Tsinghua University, etc.2023[108]
13~161.451.52×101215Fudan University, etc.2023[109]
14.53.511×10877Changchun University of Science and Technology, etc2023[110]
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量子级联技术研究进展:从光源到探测
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杨超 1 , 李泰澎 2 , 黄宝玉 2 , 李愽乐 2 , 张盛楠 1 , 黄彦 1 , 王兆刚 1 , 史青 1 , 尹玉刚 1 , 彭泳卿 1 , 李晓干 2
遥测遥控 | 综述与评论 2024,45(3): 1-23
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遥测遥控 | 综述与评论 2024, 45(3): 1-23
量子级联技术研究进展:从光源到探测
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杨超1, 李泰澎2, 黄宝玉2, 李愽乐2, 张盛楠1, 黄彦1, 王兆刚1, 史青1, 尹玉刚1, 彭泳卿1, 李晓干2
作者信息
  • 1北京遥测技术研究所 北京 100076
  • 2大连理工大学集成电路学院 大连 116024
  • 杨超 1988年生,博士,工程师。

    李泰澎 2000年生,硕士研究生。

    黄宝玉 1992年生,讲师,硕士生导师。

    李愽乐 2001年生,硕士研究生。

    张盛楠 1994年生,博士后,工程师。

    黄彦 1990年生,博士,高级工程师。

    王兆刚 1990年生,博士,高级工程师。

    史青 1982年生,博士,研究员。

    尹玉刚 1982年生,硕士,研究员。

    彭泳卿 1980年生,博士,研究员。

    李晓干 1976年生,教授,博士生导师。

Research Progress of Quantum Cascade Technology: From Light to Detection
Chao YANG1, Taipeng LI2, Baoyu HUANG2, Bole LI2, Shengnan ZHANG1, Yan HUANG1, Zhaogang WANG1, Qing SHI1, Yugang YIN1, Yongqing PENG1, Xiaogan LI2
Affiliations
  • 1.Beijing Research Institute of Telemetry, Beijing 100076, China
  • 2.School of Integrated Circuits, Dalian University of Technology, Dalian 116024, China
出版时间: 2024-05-15 doi: 10.12347/j.ycyk.20231024001
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量子级联技术基于多量子阱或超晶格结构中的子带跃迁和共振隧穿理论,既可以产生光源,又可以探测光信号,是量子级联激光器(QCL)和量子级联探测器(QCD)的理论基石,在检测、遥感、通信、雷达等领域具有广泛的应用前景。经过最近三十年的研究,量子级联技术在基础研究、产品性能以及应用系统研发和场景试验方面都取得了重大进展。本文首先简要介绍了量子级联技术的原理和发展历史,随后阐述了量子级联器件子带能级结构和电子输运动力学计算思路,接着重点综述了量子级联技术的研究进展,包括中远红外高功率QCL、中远红外宽调谐QCL、太赫兹QCL、高性能QCD,以及QCL和QCD的单芯片光子集成方面的内容,最后介绍了QCL和QCD的产品与应用情况。

量子级联  /  激光器  /  探测器  /  集成  /  进展

Quantum cascade technology, based on resonant tunneling and intersubband transitions in a multiple-quantum well or superlattice structure can generate light source and detect optical signals, it is the theoretical cornerstone of quantum cascade laser(QCL) and quantum cascade detector (QCD), which has wide application prospect in detection, remote sensing, communication, ra-dar, and other fields. After three decades of research, quantum cascade technology has made significant progress in basic research,product performance, application system research and scene testing. In this paper, the principle and development history of quantum cascade technology are briefly introduced first. Subsequently, the calculation approaches of intersubband energy level structure and electron transport dynamics in quantum cascade devices are elaborated. Next, the research progress of quantum cascade technology is mainly reviewed, including mid- and far-infrared high power QCL, mid-and far-infrared widely tunable QCL, terahertz QCL, high performance QCD, and single-chip photonic integration of QCL and QCD. Finally, the commercially available QCL and QCD products, as well as their application status, are introduced.

Quantum cascade  /  Laser  /  Detector  /  Integration  /  Progress
杨超, 李泰澎, 黄宝玉, 李愽乐, 张盛楠, 黄彦, 王兆刚, 史青, 尹玉刚, 彭泳卿, 李晓干. 量子级联技术研究进展:从光源到探测. 遥测遥控, 2024 , 45 (3) : 1 -23 . DOI: 10.12347/j.ycyk.20231024001
Chao YANG, Taipeng LI, Baoyu HUANG, Bole LI, Shengnan ZHANG, Yan HUANG, Zhaogang WANG, Qing SHI, Yugang YIN, Yongqing PENG, Xiaogan LI. Research Progress of Quantum Cascade Technology: From Light to Detection[J]. Journal of Telemetry, Tracking and Command, 2024 , 45 (3) : 1 -23 . DOI: 10.12347/j.ycyk.20231024001
量子级联技术属于量子科技的重要范畴,基于多量子阱或超晶格结构中的子带跃迁和共振隧穿理论,不仅可以实现从“电到光”的光源功能,还可以实现“光到电”的探测功能[1-7]。由量子级联技术所研发的典型产品包括量子级联激光器(Quantum Cascade Laser, QCL)和量子级联探测器(Quantum Cascade Detector, QCD),其中QCL可以产生红外到太赫兹(THz)波段的激光光源,而QCD可以探测红外到太赫兹波段的电磁波信号[2,6]。QCL的激光功能和QCD的探测功能取决于有源区量子阱和势垒材料的厚度和组分,其决定了有源层导带中的子带能级位置,从而可以实现对激射波长和探测波长的调控。相比于传统的固体激光器等,QCL具有尺寸小、重量轻、激射波长可调谐以及电光转换效率高等诸多优点[2,8,9];而与传统的红外探测器相比,QCD具有小型化、无暗电流、探测波长覆盖范围宽以及高频响应特性等诸多优点[6,10,11]。QCL和QCD的优异品质使其在微量气体检测、医疗诊断、红外成像、定向红外对抗、天基红外预警等民用和军用领域具有广阔的应用前景[8-13]
量子级联技术的理论萌芽起源于前苏联,之后在1994年,美国Bell实验室研制出世界上首台中红外QCL[14],随后,第一台太赫兹QCL[15]和第一台QCD相继问世[16]。经过最近三十年的不断研究,量子级联技术在激光功能和探测功能基础研发方面已经取得了一系列突破,性能指标参数如工作温度、光束质量、波长拓展、调谐范围、输出功率、探测率等已取得大幅提升和改善[8,11,13]。例如,中红外QCL从最初仅能在低温10 K下工作到现在可以在高温408 K下工作[14,17],输出功率从低温脉冲模式下的8.5 mW增加到现在室温连续输出下的5.6 W[14,18];太赫兹QCL从最初可在低温8 K下工作到现在可在最高261 K下工作[15,19],输出功率从低温脉冲模式下的2 mW增加到现在温度为58 K脉冲输出下的2.03 W[15,20];QCD的响应率从早期温度为50 K下的35 mA/W增加到现在温度为295 K下的85 mA/W[16,21]。诸如此类芯片结构设计、高品质的外延材料生长以及芯片流片工艺等方面的突破,尤其是有源层能带设计、波导设计、光耦合设计等芯片结构设计方面的持续改进,有力地促进了激光输出性能和探测性能的提高[2,6,8,9,13]。量子级联技术的持续突破最终推动量子级联器件产品的应用[22-24],从而促进了基于量子级联产品的应用系统研发和试验研究,包括气体检测、激光通信、生物医疗以及定向红外对抗等领域[12,25,26]
本文首先简要介绍了量子级联技术的原理和发展历史,其次阐述了量子级联器件子带能级结构和电子输运动力学计算方法,再次针对量子级联技术在基础研发方面的研究进展进行了重点综述,具体包括中远红外高功率QCL、中远红外宽调谐QCL、太赫兹QCL、高性能QCD,以及QCL和QCD的单芯片光子集成等五方面内容,最后介绍了QCL和QCD的产品与应用情况。
量子级联技术引领了中红外到太赫兹波段的光源和探测技术革命。本综述在更深层面上阐述了量子级联技术,希望借此促进量子级联技术的研究、发展和应用。
量子级联技术的本质是研究微观粒子在具有级联特征的量子维度和尺寸结构中的热力学和动力学行为。“量子”即组成有源层结构的材料,由处于纳米或原子级别的多量子阱构成。因为量子尺寸效应导致量子阱中产生了一系列不连续的子带能级,电子只能占据这些不连续的能级并发生跃迁和量子隧穿[1,27,28],可以通过改变量子阱层和势垒层材料的厚度来调控子带能级的位置,从而调节激光激射波长或探测吸收波长。“级联”即把包括有源区和弛豫区的基础结构单元依次连接起来,通过合理设计子带能级或微带结构的位置,电子便可以在这些重复的基础结构单元里连续不断地发生能级跃迁和隧穿势垒的行为,导致产生倍增的“电到光”信号,从而显著提高量子效率,获得更高的激光输出性能。图1为能带原理示意图。
基于量子级联技术所研发的典型产品包括量子级联激光器QCL和量子级联探测器QCD。图1(a)中,该能带结构中的每个级联周期均包括一个有源区/辐射区和一个注入区/弛豫区,在外加偏压下,电子通过共振隧穿从注入区最后一个势垒进入到有源区的上能级,紧接着从上能级跃迁至下能级并激发出光子,下能级的电子通过与纵向光学声子相互作用而被抽运到注入区,经由注入区多个势垒的弛豫减速作用后,最终又一次进入到下一个毗连级联结构中的有源区上能级,继续重复着辐射跃迁和共振隧穿的行为[29,30]图1(b)中,该能带结构中的每个级联周期由有源区/吸收区和弛豫区/级联输运区构成,在特定波段的电磁波照射下,处于吸收区基态的电子在吸收光子能量后从低能级被激发到高能级,然后借助共振隧穿进入弛豫区,随即电子通过与纵向光学声子的相互作用而逐渐“滑下声子台阶”,最终又一次经过弛豫,到了下一个毗邻级联结构中的有源区基态能级,来继续吸收光子并重复进行跃迁行为[10,31]。由“电到光(QCL)”还是“光到电(QCD)”,根本上取决于量子级联材料中的能带结构,其又由多量子阱或超晶格的结构特性(如厚度、组分等)所决定。
量子级联技术的研究经历了以下几个发展阶段:
① 理论与实验探索阶段(1971~1994年)。1971年,前苏联的Kazarinov和Suris最早提出了量子级联技术的理论基础[30]。但是,由于在理论上和实验技术上的难点导致QCL的研发遇到较大困难,进展较为缓慢。直到1994年,由于能带理论和量子材料生长技术上的突破,美国Bell实验室的J. Faist等人研制出了世界首台中红外QCL[14]。尽管当时仅能够在极低温的10 K下产生毫瓦量级的中红外激光,但它的诞生意味着量子级联技术实现了里程碑式的突破。
② 技术不断创新与样机研发阶段(1995~2010年)。基于能带工程,多样化的量子级联有源区结构被不断设计出来,包括双声子共振设计、束缚态-连续态设计以及共振声子设计等,由此产生了多元化的量子级联样机研发成果,诞生了第一台中红外室温连续QCL(2002年,瑞士)[32]、第一台太赫兹QCL(2002年,意大利和英国)[15],以及第一台以探测为目的QCD(2004年,法国)[16]等。
③ 产品性能不断提高与应用场景探索阶段(2010年至今)。随着理论设计(电、光、热方面)、外延技术以及器件制造技术的不断成熟,国内外研发的QCL和QCD产品的性能逐渐提高,向着更高工作温度[11,33,34]、更高输出功率[18,35,36]、更宽调谐范围[37-39]、更多的工作波长选择[6,8,13]以及更高的响应率和探测率[11,21,40]等性能指标上逐步迈进。与此同时,针对QCL和QCD产品的应用场景试验探索也逐渐展开,包括检测、通信、探测以及红外对抗等场景[12,23,41,42]
量子级联器件(QCL和QCD)的子带能级结构和电子输运动力学从根本上决定了器件的输出和探测性能,因此对子带能级结构和电子输运动力学这两部分的建模和求解就显得尤为关键。
量子级联激光器和量子级联探测器的子带能级结构产生原理相一致,这里重点介绍器件结构中量子阱/超晶格材料的子带能级结构的理论模型和求解思路[30,43,44]。QCL有源区由交替生长的不同半导体材料薄层组成,在导带中形成了量子阱/势垒,因此,电势与有效质量会在QCL的外延生长方向上变化(这里用z表示),而xy是指面内方向。QCL异质结构通常在Ben Daniel-Duke模型框架中处理,此模型仅考虑发生辐射跃迁和载流子输运的导带,这种近似情况下,定态薛定谔方程可写为:
ψ为波函数,E为本征能量,m//是面内有效质量,m*为生长方向即垂直于外延层的有效质量,V为电势。对于束缚态,波函数通常为归一化的,即。由于V和有效质量仅取决于z方向,因此可有:
ψ(x,y,z)=S-1/2ψk(z)exp(ikxx+ikyy)
其中,S为面内横截面积,k=[kx,ky]T为平面内波矢量。S-1/2在式(2)中用来获得归一化条件:∫|ψk|2dz=1。将式(2)代入式(1)中得到Ben Daniel-Duke模型:
其中波函数ψk(z)和能量Ek取决于平面内电子的运动,即与k相关。通过忽略面内有效质量m//z的依赖性,可以解耦得到常规形式的一维薛定谔方程:
本征能量E取决于一维z方向上的电子约束且与总能量有关(Ek=E+Ekin)。其中,
Ekin为电子在平面内自由运动而产生的动能。有效质量不仅取决于材料成分[45],还取决于晶格温度和掺杂浓度[46]。后一种影响往往在QCL中起次要作用,因此通常被忽略。对于应变QCL结构,有效质量还受到不同半导体材料之间的晶格失配的影响,导致(m//m*)[47]
一维有效质量薛定谔方程的求解需要通过可靠的数值解方法实现,而且高效率的计算和简单的实现方式也十分重要,因为QCL的设计和优化任务需要执行大量的模拟计算。常用的数值方法包括传递矩阵法[48]和有限差分法[49]。这两种方法各有优缺点。传递矩阵法可较易考虑非抛物线等效应,还可精确处理QCL异质结构中量子势垒和量子阱之间的电位阶跃问题。有限差分法由于舍入误差导致的指数级计算量激增,可能会对多势垒或扩展势垒产生数值不稳定性,不过这个问题可以通过使用散射矩阵方法等解决[50]图2给出了传递矩阵法和有限差分法的示意图。
在最低阶情况下,可以通过自洽求解方程(4)和泊松方程来考虑电子间的相互作用[51]
在式(6)中,ϵ(z)是随半导体成分变化的介电常数,e表示元电荷。方程(6)的右侧对应于QCL异质结构中由具有浓度nD(z)的正电荷施主和电子引起的空间电荷ρ,其中是具有波函数ψ(z)的能级i的电子面电荷密度。
方程(6)可以应用有限差分法来求解。可建立:
且有
并且
然后在单个QCL周期zЄ[z0+Lp]内求解方程(6),其中网格点zn(n=0…P)应与求解薛定谔方程(4)的网格重合。应用边界条件,方程(6)可以写成矩阵方程,其中ρ分别表示具有元素ρn的向量,n=1…(P-1),M为具有非零元素Mn,n=,Mn,n-1=-,Mn,n+1=的矩阵,则可以使用三对角方程系统的算法来高效解决这个方程[52]
在薛定谔方程式(4)中,总势能V=V0+,其中必须通过求解泊松方程(6)来获得。另一方面,在方程(6)中的波函数ψi必须从方程(4)中确定。在计算上,最初假设=0,通过迭代求解薛定谔-泊松方程,直到对ψiEi的结果收敛[51]。如果是通过自洽的载流子输运模拟获得,则需要迭代进行载流子输运模拟和薛定谔-泊松系统的数值求解,直到获得收敛结果。这样的模拟计算方法被称为self-consistent(自洽)方法[53]
量子级联器件的电子输运动力学较为复杂,因为涉及到电子在耦合的多量子阱或超晶格结构中的辐射跃迁、共振隧穿以及各种散射等微观物理过程。通常的求解模型或方法包括了经典的速率方程模型、半经典的密度矩阵方法、蒙特卡洛模拟,以及基于全量子计算的非平衡格林函数方法[54]。速率方程模型求解过程较为简单而且计算结果相对准确,是求解量子级联器件电子输运动力学的有效手段[43,44,55,56]。对于QCL而言,速率方程模型能够揭示一些最重要的器件性能参数,比如微分增益和内量子效率,如图3所示,下文进行简要介绍[55,57,58]
图3为一个典型的中红外QCL的有源区结构示意图。流入有源区的总电流密度为J,其中大部分是通过具有注入效率为ηinj的隧穿效应来到达上激射能级,其余则被注入至下激射能级。激光上激射能级和下激射能级的粒子数分别用NuNl表示。τuτlτul分别表示电子从上激射能级的散射寿命、从下激射能级的散射寿命和从上激射能级散射到下激射能级的寿命。需要注意的是,因为注入区微带结构内有许多能级,所以τul的散射过程是τu的散射过程中的一部分。受激辐射引起的子带间跃迁用一个包含光子密度δ的项表示。该项与粒子数反转Nu-Nl和增益系数ξ成正比。增益系数与偶极矩元z的平方及线宽γ的倒数成正比,可以表示为:
式中的neff为器件的有效折射率,λ是波长,e为电子电荷,ε0为真空介电常数。
低于阈值的速率方程,也就是不含受激发射项,是根据如下情况构建,即某一能级的粒子数变化率等于进入该能级的散射速率与离开该能级的散射速率之差。因此,对应上激射能级和下激射能级的速率方程可表示为:
其中,L表示一个QCL级联周期的长度。
对于阈值以上的计算,需要将受激辐射项加入到方程(11)和方程(12)中,得到:
此外,考虑到光子产生和泯灭的平衡,可以构造类似光子密度速率方程:
其中,αtotal为系统总损耗,Γ为光限制因子。稳态方程如下:
同样的,需要把除了NuNlδ外的所有参数都当作已知,然后去求解方程(16),得到的是:
其中,ηinter为内量子效率,阈值电流密度Jth表示为:
阈值以上的粒子数反转可以由方程(17)和方程(18)得到,即为:
可知,DN独立于J。在阈值点的上激射能级粒子数为:
结合方程(22)和方程(17)可以得到:
输出功率P与光子密度δ和镜面损耗αm成正比:
其中,NA分别表示QCL级联周期数和电流流经的截面面积,即腔长与脊宽的乘积。ω为光子频率。
将方程(19)代入方程(24),将总损耗atotal视作镜面损耗am与波导损耗aw之和,得到斜率效率表达式为:
方程(25)最终揭示了内量子效率的物理意义,它表示在所有参与输运的电子中,参与光子发射的电子的比例,也可以解释为每个发射周期中每个注入电子所发射的光子数。
一般来说,表征QCD电子输运的方法有很多种,但因为载流子的捕获过程是由不同的散射过程决定的,且逃逸过程也是由强烈依赖温度的散射过程而决定[59-61],所以散射过程在很大程度上影响了载流子捕获和逃逸概率,因此,需要很精确的方程模型来表征QCD。和QCL类似,QCD也采用经典的速率方程模式,因为它可以处理子带能级上粒子数的变化率,并且考虑了QCD结构内部受不同散射过程影响下的所有可能的载流子输运机制[6,62,63]
QCD电子输运研究前需要精确计算能量状态和与状态相关的波函数,要通过求解薛定谔-泊松自洽方程组得到。泊松方程考虑了量子阱的掺杂,可以给出相关能带结构的精确数值求解过程。在薛定谔方程中考虑了温度对能带结构的影响,采用Varshni关系式计算对温度依赖的导带偏移量,将薛定谔方程中的导带电子有效质量考虑为与能量相关的参数来处理导带的非抛物线效应[64]
电流响应率可以定义为每单位入射辐射的光功率密度产生的输出光电流密度。响应率可以写为:
其中,Jphoto为输出光电流密度,Pin为入射辐射在探测器表面的功率密度。
为了模拟载流子在结构中的运输,可以考虑Kargan等人的速率方程模型方法[65]。目前的QCD结构是多周期结构,每个周期包含多个量子阱,每个量子阱有多个束缚能态。因此,特定能量状态中的载流子动力学不仅受与该周期相关的其它能量状态的影响,还受与左右相邻周期相关的能量状态的影响。此外,QCD结构表现出平移对称性。因此,仅用一个相邻周期即可描述特定周期的整体载流子动力学,这里取右邻周期。此外,由于结构的周期性,不同周期的相同能量状态的载流子动力学将是相同的。图4给出了周期A中特定能级5的载流子动力学以及该状态相关的散射过程,处于1能级的电子吸收光子能量后(红色波浪箭头表示)跃迁激发到能级5,然后经过共振隧穿进入阶梯能级进行输运,曲线黑箭头表示共振隧穿输运过程,实线直箭头表示子带间和子带内的散射过程,该过程中的电子不仅散射到A周期的阶梯能级,而且还散射到B周期的阶梯能级上,虚线直箭头表示周期A对周期B中特定能级(5+)的影响。
与某一特定周期的能级有关的速率方程可以用如下方程组表示:
其中,n表示由与QCD中周期A关联的ij以及与周期A毗连的周期B关联的i+j+指定的特定能态的二维电子密度。Jtunnel是两个空间间隔为d的能态之间的共振隧穿电流密度,其表达式为:
其中,Δd为失谐能,ћϖ为耦合能,L为单周期长度,kB为玻尔兹曼常数,T为器件温度,γ为均匀散射势。考虑单周期内的速率方程中,薄层面密度转换为体积密度时,分母中出现了系数L。QCD周期内的总状态数用Ω表示,一个电子的总子带间跃迁速率可以表示为
其中,表示总非辐射散射速率,是辐射跃迁速率,其计算公式为[65]:
其中,ћωpht为光子能量,ϕ为光通量,φ是入射辐射相对于生长z方向的偏振角,ϑ为状态ij之间光跃迁的半高宽。系统中控制载流子输运动力学的主要非辐射散射过程是电子-电子(e-e)散射、电子-纵向光学声子(e-LO)散射、电子-界面粗糙度散射、以及电子-离化杂质散射[66,67]。对于能量状态间隔很小且具有较高能级粒子数的系统,电子-电子散射过程较为重要[68]。在这里,忽略了电子-电子散射过程,因为能级之间的能量间隔较大。由于量子级联系统中拥有较多的界面,因此电子-界面粗糙度散射不能被忽略[69]
e-LO声子散射速率可以表示为[70]
其中,Θ为Heaviside函数,ki为子带 i 中电子的平面波矢量,kz是声子波矢量。这里的
而且有
其中,ωphn为LO声子的角频率,ε为高频介电常数,εstatic为静态介电常数。减号表示声子吸收过程,加号表示发射过程。声子占据数用N0=表示,方程中的其它项含义可参考相关文献[71]
总的e-LO声子散射率为:
电子-离化杂质散射速率可以表示为[67,72]
这里的
其中
N(Z)是Z位置电离杂质的体积密度。
以高斯自相关函数表征的界面粗糙度分布[67],平均粗糙度高度为D0、粗糙度横向大小为Λ的电子-界面粗糙度散射速率为[72]
方程中V0是界面电势高度。对子带上载流子热分布的散射率进行平均,可以得到两个能级之间的平均载流子散射速率:
其中,Eini是初始态的量子化能量,f为Fermi-Dirac分布函数。对于e-LO声子散射,Estatic=ћωphn。对于电子-离化杂质散射和电子-界面粗糙度散射,Estatic=0。发射过程用减号表示,吸收过程用加号表示。
因此,两个能级之间的总非辐射散射速率可表示为:
可以利用四阶的Runge-Kutta方法对稳态的速率方程进行求解以获得子带粒子数。
在光照下正向流动的净电流给出了总的光电流。为了计算在两个连续的QCD周期之间的净电流,可考虑一个假想的参考平面(见图4),并且净电流取为通过参考平面的正向电流和反向电流之间的差值。因此,总输出光电流密度可以写为[65]
由此,可计算出QCD的响应率,进而计算出比探测率等参数。
QCL芯片有源区能带结构和电子输运特性从根本上决定了激光器电光转换效率和输出功率的极限。能带结构方面需要考虑子带能级的位置和数量,而电子输运方面需要考虑共振隧穿、注入效率、辐射跃迁、散射速率、载流子的热回填等因素。迄今为止,研究人员已经设计开发出二十余种有源区结构,包括单声子共振结构、超晶格结构、双声子共振结构等[9]。在这些有源区结构中,双声子共振结构较为经典。2008年,美国西北大学的Y. Bai等人基于该有源区能带结构,在4.6 μm中波红外波段下,首次实现了QCL瓦级光功率输出[73]。与更早期的单声子共振结构相比,双声子共振结构采用了包含有四个量子阱的有源区设计思路,最大特点是在下能级位置设置了三个子带能级,借助连续释放两个纵向光学声子来快速实现对下能级电子的抽空,该结构具有较高的注入效率,并能够抑制载流子的热回填[29]。然而,双声子共振有源区的设计也有明显缺点:由于下能级子带能级之间的能量差需要严格与纵向光学声子的能量相互匹配,因此,有源区材料的生长厚度必须严格与设计值相一致,也即该结构对厚度容错率较低。为了实现更高的输出功率,目前已经开发出一些新颖的有源区结构,包括非共振抽取有源区结构、浅阱高势垒有源区结构以及双阱有源区结构[9]。如图5(a)所示,非共振抽取有源区结构移除了传统双声子共振设计中两个声子共振的约束限制,而通过在下能级的下方设置出几个平行的子带能级来提供较低的下能级寿命,同样可以有效地促进粒子数反转[56,74]。而且,因为无需双声子共振条件,所以便于调控上能级以上的寄生能级,通过增加上能级和寄生能级之间的能量差,可以有效抑制上能级载流子的热逃逸,最终提高电子的辐射跃迁效率。图5(b)为浅阱高势垒有源区结构的导带结构和波函数图,该结构的设计核心是引入多种不同组分的量子阱和势垒层,尤其是利用具有高势垒的AlAs砷化铝层来强烈抑制上能级载流子的热逃逸,提高了注入效率[2,75]图5(c)为双阱有源区结构导带结构和波函数图,在该结构中通过改变注入势垒的厚度来调控注入区基态能级和毗邻有源区上能级的耦合能量间隔,从而提高注入效率。此外,通过去除有源区中第一个较薄的量子阱和势垒对,有助于增加上能级和寄生能级间的能量差值,抑制了载流子的热逃逸[56,76]
QCL增益有源层的周围需要被光波导材料包覆以实现对光场的限制,从而降低波导损失,获得较高的光模限制因子。在QCL外延生长方向,通过改变平板波导中各层材料的掺杂浓度和厚度等参数来对波导结构进行优化。在早期,美国Bell实验室研究人员曾使用波导包覆层(InAlAs)并结合波导限制层(InGaAs)的设计思路来对光场进行限制[14],后来他们意识到磷化铟(InP)材料的折射率要低于InAlAs的折射率,非常适合作为波导包覆层的材料,而且磷化铟热导率相对较高,可以快速移除激光芯片的自生热,所以逐渐采用磷化铟材料作为波导包覆层,这进一步增加了QCL的输出功率并提高了工作温度值[77,78]。将有源层包覆在上、下波导限制层InGaAs的这种波导结构设计较为经典,可以实现较好的光模限制效果。考虑到InGaAs材料热导率比较低,因此美国西北大学等单位进一步将InGaAs也替换为InP,构成了全InP材料的波导结构,在有效降低激光器芯片热阻的同时又能得到很高的光模限制因子值[18,55,56]。当前,大多数高性能QCL通常采用全InP材料包覆的波导结构设计思路。在QCL脊波导两侧方向,通常采用选择性二次外延技术在脊波导两侧生长半绝缘掺Fe(铁)的InP材料,相比于传统SiO2或Si3N4绝缘材料,InP不仅可以更好地对横向光场进行限制,降低光波导损失,还有利于促进横向散热,提高芯片的散热能力[9]。在QCL腔面方向,通常需要在后腔面和前腔面分别蒸镀高反膜和增透膜来减小阈值电流密度值并增加输出功率值。值得注意的是,增透膜的反射率并不是越小越好,而是存在一个较优的数值以获得较佳的腔面损耗,从而平衡阈值电流密度和电光转换效率这两个参数的关系。
QCL芯片通常需要被注入较大的电功率,再加上电光转换效率较低,从而导致QCL芯片内部产热量巨大,造成芯片核温度较高。芯片温度的升高加剧了有源区上能级载流子的热逃逸和下能级载流子的热回填,从而减小了粒子数反转和增益,最终增加阈值电流密度、减小电光转换效率和输出功率。针对激光芯片的散热设计,首先,需要从源头上提高电光转换效率,降低废热产生量。电光转换效率由四种不同的分效率构成,分别是内量子效率、电压效率、电气效率以及光学效率,这些分效率主要是依赖于对芯片有源层和波导结构的设计和优化[2,55]。其次,需要结合多种散热手段来促进芯片的散热,包括采用电镀厚金层、倒装焊接、高热导率的金刚石基板以及选区二次外延掩埋脊波导等技术手段来降低器件热阻并增加散热通道,进而有效地促进激光器芯片有源层热量的导出[9]。此外,还可以采用微流控等外部冷却技术来促进激光芯片的散热。高效的散热设计有利于实现QCL室温连续工作,并提高激光输出功率和稳定性。
2002年,瑞士纳沙泰尔大学J. Faist教授的团队成功研制出了世界首台能够室温连续激射、输出光功率为10 mW的QCL[32],这是一个里程碑式的突破。此后,实现更高的QCL输出光功率和电光转换效率便成为人们在QCL研究方面最主要的工作方向和突破目标。图6汇总了近些年国内外研究人员研制的4~5 μm中波红外和7~12 μm长波红外单管QCL在室温下连续工作的输出功率[9]。目前,美国西北大学在高功率QCL等领域的研究处于世界领先地位。2020年,美国西北大学继续在中波红外和长波红外单管芯高功率QCL上取得突破,并获得了迄今为止最高的输出光功率和电光转换效率,其中,在4.9 μm中波红外波段可实现室温连续5.6 W的输出光功率以及22%的连续电光转换效率[18],在8.3 μm长波红外波段可实现室温连续3.4 W的输出光功率以及13%的连续电光转换效率[36]。此外,相当多的国内外机构都可实现室温连续瓦级输出功率和较高的电光转换效率。中长波红外QCL输出功率和电光转换效率性能的不断提高可归功于在芯片结构设计、高质量的外延材料生长,以及高散热特性器件的制造工艺方面的改进和突破,其中最为关键的即是采用了新颖的有源区设计[9]。先进的有源区设计可以提高内量子效率和电压效率,从而有助于提高激光芯片的电光转换效率以及输出光功率。
除了高功率室温连续QCL,高功率室温脉冲QCL也是人们研究的方向。高功率室温脉冲QCL可以通过基于宽脊的功率放大技术来实现,例如2009年,美国西北大学的Bai等人研制了具有400 μm脊宽的QCL,其发射波长为4.45 μm,在室温脉冲模式下可实现120 W的峰值输出功率[79]。此外,还可以利用基于多个QCL管芯阵列的合束技术来实现功率放大,从而获得更高的输出功率。2018年,美国西北大学的Zhou等人报道了发射波长为4.8 μm的具有单模、16通道光学相控阵的高功率QCL集成器件,该集成器件由一个分布式反馈部分、一个高效树形阵列多模干涉功率分配器和一个16 通道放大器阵列构成(如图7所示),在15 ℃下可实现30 W的脉冲峰值输出功率[80]。2019年,Zhou等人同样基于树形阵列多模干涉器研制出了具有八个单管芯的高功率锁相QCL阵列,其发射波长为8 μm,可在室温下连续工作,输出功率高达8.2 W[81]。2023年,Wang等人研制了4.6 μm的QCL阵列,可得到12 W的峰值光功率[82]
中远红外宽调谐QCL在多组分气体检测等领域具有重要的应用前景。通过QCL的外部调制技术和QCL芯片的有源区设计可以实现量子级联激光器宽波段调谐工作。QCL外部调制技术可以采用分布反馈DFB-QCL阵列、单片多驱QCL,以及外腔EC-QCL等手段来实现宽调谐机制[2,8]。外腔EC调制技术可实现较宽的调谐范围,但需要额外的光学元件,因此其体积较大导致其调谐速度也受到限制;而分布反馈DFB激光阵列具有紧凑、单片集成以及调谐速度快等优点,但制造工艺较复杂[2,8,37]
除了外部调谐机制,还需要能够获得宽增益谱的QCL芯片有源区结构设计来实现更宽的调谐范围。迄今,所发明和设计的宽谱QCL有源区结构包括束缚-连续态跃迁结构、双重上能级态结构以及异型多核级联有源区结构[2,8]图8(a)为束缚-连续态跃迁结构,该结构由Faist等人在2001年所设计,借助下能级态的啁啾超晶格所构成的微带/连续态结构,下能级态的连续带中会产生较多的能级态,上能级中的电子可以跃迁到下能级微带中不同的子带能级态中,从而可以获得相对较宽的量子级联激射光谱[83,84]。2011年,日本滨松光子学公司的Fujita等人报道了一种双重上能级态到多重下能级态的有源区能带结构设计,如图8(b)所示,这种能带结构可以提供众多跃迁组合方式,实现不同的激射波长,最终获得了高达600 cm-1的宽增益谱[38]。2015年,美国西北大学的Bandyo-padhyay等人研发出了基于六个子核堆垛结构的异型多核级联有源区宽谱激射结构,如图9(a)所示,增益模拟曲线见图9(b),该有源区结构可实现6~10 μm的波长调谐范围,波数调谐范围可实现600 cm-1[85]。2015年,美国西北大学的Bandyopad-hyay等人再次基于异型多核级联有源区结构并通过制作分布反馈DFB激光阵列来获得迄今最高的超宽谱量子级联激光器,发射波长范围在5.9~10.9 μm(见图9(c)),调谐范围高达760 cm-1[37]。2016年,美国西北大学的Zhou等人同样采用异型多核级联有源区结构,并制作成了采样光栅分布反馈(SGDFB)结构,也可实现520 cm-1的调谐范围[39]。异型多核级联有源区结构包含了具有不同输出波段的多个子核,因此可实现更宽的波长调谐范围。
太赫兹波是处于红外和微波之间的电磁波,在太赫兹光谱检测、安全检查、无线通信、医疗诊断、太赫兹成像等领域具有重要的需求和应用前景。然而,处于1~10 THz频率范围内的电磁波通常被称为“太赫兹带隙(THz gap)”,这是由于传统的光电器件很难产生该频段的太赫兹辐射源。2002年,Köhler等人首次研发出了太赫兹QCL,成功弥补了这段“太赫兹带隙”[15]
相比于中红外QCL,太赫兹QCL的激射波长更长,因此能量更小,导致上下能级差较小,且通常要小于纵向光学声子的能量(GaAs,36.5 meV),这导致上能级载流子会受到热激发的纵向光学声子的散射作用而产生逃逸,从而降低粒子数反转。较小的上下能级差是太赫兹QCL有源区设计的关键难点。早期的太赫兹QCL有源区设计可以借鉴中红外QCL有源区设计思路,包括采用了啁啾超晶格结构和束缚-连续有源区结构,但是这两种有源区结构都通过发射纵向光学声子来促进下能级电子抽运到注入能级,很难避免上能级中的电子也被散射掉[86]。为了进一步改善太赫兹QCL的性能,已研究出共振声子结构、散射辅助结构以及两阱直接声子结构等新颖的有源区结构[4,86]图10(a)为共振声子结构示意图,其具有三个量子阱,通过共振隧穿过程电子被直接注入到上能级态,经过辐射跃迁进入下能级态,下能级态上的电子同样经过共振隧穿进入到抽运态,随即再通过纵向光学声子的散射作用而再次进入注入态。共振声子结构设计可以选择性注入电子到上能级态并从下能级态中抽运电子来实现较高的粒子数反转。然而,共振声子结构的缺点是存在着不希望的共振隧穿通道和载流子逃逸路径,从而影响太赫兹QCL的输出性能[87,88]图10(b)为散射辅助结构示意图,在该结构中电子仍可以通过共振隧穿过程进入到抽运态,但是最主要的特征是电子需要通过直接的纵向光学声子散射作用从注入态进入到上能级态。散射辅助结构设计具有更高的选择性来注入到上能级,且在小于3 THz的较低频率下具有较宽的动力学范围[89]图10(c)两阱直接声子结构示意图,该结构中的每个量子级联周期具有最少的层数,即仅包含两个量子阱和两个势垒层。相比于共振声子结构设计,由于在两阱直接声子结构中的载流子输运仅依赖于单个共振隧穿过程,因而更不容易受到设计和生长因素的影响。此外,相比于散射辅助结构设计,两阱直接声子结构的每个量子级联周期少了一个纵向光学声子散射过程,因此会产生更少的晶格热。两阱直接声子结构不仅量子结构计算和优化相对容易,而且由于有源层可以容纳更多的级联周期数目,从而可以获得更高的光增益和器件温度特性[4,33]。由于太赫兹QCL和中红外QCL都会受到载流子热逃逸到更高寄生能级和连续能级的影响,因此,除了对有源区量子阱的数量和子带能级的位置进行调控以外,还可以通过提高势垒能带的带边来抑制载流子的热逃逸,从而改善输出性能。
太赫兹QCL的波导结构对提高其输出性能起着重要作用。在2002年,首个太赫兹QCL采用了半绝缘的表面等离子体波导结构,从下往上依次是半绝缘的GaAs衬底、高掺杂的接触层、有源层、金属层[15]。由于具有较低的面反射率,表面等离子体波导结构的优点是可以产生较好的光束质量和较高的输出功率。但是,表面等离子体波导结构中的光模通常会延伸扩展到半绝缘的GaAs衬底,因而会导致器件产生较高的自由载流子损耗[4,13]。为了改善光模限制因子,太赫兹QCL采用了双金属的波导结构,通过金属晶圆键合的方法将有源层加在两个金属层之间。相比于表面等离子体波导结构,双面金属波导结构的光模限制因子接近1,这有利于实现较低的阈值电流密度和高工作温度的太赫兹QCL[4,13]。此外,金属波导结构的金属选择对性能也有影响,利用Cu来替换Au或者Ta来替换粘附层Ti有利于获得更高的工作温度[90,91]
自从太赫兹QCL问世以来,部分性能暂时还不如更为成熟的中红外QCL,但其输出性能在不断提高。影响太赫兹QCL性能的关键参数包括激射频率、频率调谐范围、输出功率以及工作温度[4,13]。在激射频率方面,目前可实现1.2~5.4 THz的激射频率范围[4,13]。在频率调谐范围方面,2015年,瑞士苏黎世联邦理工学院Rosch等人基于异型多核级联有源区结构设计思路研制出超宽谱太赫兹QCL,激射频率可连续从1.64 THz调谐到3.35 THz,激射谱宽高达1.71 THz[92]。2019年,美国加州大学洛杉矶分校的Curwen等人研制出了基于量子级联超构表面的垂直腔面发射激光器,中心频率在3.47 THz,可实现20%的连续单模频率调谐范围(带宽达650 GHz)[93]。在输出功率方面,2017年,英国利兹大学的Li等人基于束缚态向连续态跃迁和共振声子的复合有源区结构研发出了4.4 THz QCL,在温度为10 K时的脉冲峰值功率高达2.4 W[94]。2020年,美国理海大学的Jin等人开发出了一种用于等离子体激光器中金属亚波长腔的锁相方案,基于该方案研制了锁相单模3.3 THz QCL,在温度为58 K时的脉冲峰值功率可达2.03 W[20]。除了输出功率,目前太赫兹QCL最关键的挑战就是将工作温度提高到室温。2019年,瑞士苏黎世联邦理工学院的Bosco等人通过非平衡格林函数模型系统优化了两阱有源区结构,研制出了仅采用热电制冷的5 THz QCL,该激光器的工作温度达到了210.5 K[95]。2021年,美国麻省理工学院的Khalatpour等人基于两阱直接声子有源区结构设计开发出了高功率便携式太赫兹QCL,脉冲模式下的工作温度可达250 K[33]。2023年,Khalatpour等人仍基于直接声子有源区设计进一步将太赫兹QCL的工作温度推高至261 K,是迄今为止最高的太赫兹QCL工作温度[19]。尽管目前太赫兹QCL还无法实现在室温下工作,但是采用基于双波长中红外QCL的腔内差频(Different Frequency Generation, DFG)技术所研制的DFG-THz QCL可以实现此目标。2023年,日本滨松光子学公司的Hayashi等人提出了一种可调谐非线性QCL结构,该结构使用外腔透镜耦合的Cherenkov(契伦科夫)波导,其中硅透镜紧密耦合到器件衬底,从而大幅提高太赫兹的耦合效率,由此研制出了能够在室温下工作的DFG-THz QCL,脉冲峰值功率为1 mW[19]。太赫兹QCL性能的不断提高同样归因于在有源区结构设计、波导设计、材料和外延技术以及器件工艺等方面的优化和改进,其中最关键的是采用了新颖的有源区结构设计。图11为当前不同太赫兹QCL有源区设计下的最高激射温度和激射频率之间数据关系汇总[4],可以看到工作温度超过200 K的有源区设计包括共振声子设计和两阱直接声子设计。
在国内太赫兹QCL研发方面,2016年,中国工程物理研究院王雪敏等人研制出了可在连续波工作的大功率太赫兹QCL,最大输出功率为0.23 W,工作温度为15 K[97]。2018年,中国科学院上海微系统与信息技术研究所曹俊诚研究团队实现了激射频率为4.3 THz的QCL,在10 K下的脉冲峰值功率达到1.2 W[98]。2020年,中国科学院上海技术物理研究所徐刚毅课题组研制出了太赫兹主振子功率放大器QCL,在77 K工作温度下的脉冲峰值功率达153 mW[86,99]。2023年,中国科学院半导体研究所刘峰奇课题组报道了具有倒装和掩埋异质结构的4 THz QCL,在20 K下可实现250 mW的连续波输出功率[100]
QCD的研发历史可追溯至2002年,当时瑞士纳沙泰尔大学的Hofstetter等人首次研究了基于量子级联激光器结构器件的光电探测性能,但由于该器件中的能带结构并未以探测为目的而进行设计,导致器件响应率很低[101]。2004年,法国Tha-les公司的Gendron等人对量子级联结构进行优化,首次研制出了基于量子级联能级间电子传递的光伏型子带探测器,并命名为QCD,该器件中的有源区能带结构出现了经典的光子吸收区和电子弛豫输运区[16]。此后,人们致力于开发出多元化和高性能的QCD。目前,QCD的探测波长可从近红外1 μm拓展到太赫兹波段,工作温度从10 K拓展到室温300 K,材料体系从InGaAs/InAlAs和GaAs/AlGaAs拓展到Sb基III-V族、II-VI族以及GaN材料,在室温下可实现较高的响应率和探测率、较低的噪声、较宽的宽谱响应范围、高响应速度工作[6,11,59]表1为量子级联探测器在响应率和探测率性能方面的研究进展。
多元化、高性能的QCD的成功研制主要归功于高光电效率的有源区设计和光耦合吸收效率的提升。在有源区设计方面,从最开始的垂直跃迁设计[16],发展为斜跃迁设计[104]和耦合量子阱设计[108]。对于斜跃迁设计,其有源区的光吸收跃迁发生在相邻量子阱的两个子带能级,从而产生了更大的抽运效率[104];对于耦合量子阱设计,该结构包含了两个上能级,这导致上能级到临近抽取能级的散射速率要大于上能级返回基态能级的散射速率,有力地促进了电子的正向输运迁移[108]。在光耦合设计方面,考虑到量子力学极化选择规则,通常采用的光耦合方式包括布儒斯特角耦合、45°角边入射耦合及光栅耦合[6,11,59]。布儒斯特角耦合器件的制备最简单,但是受光面在光传播方向的投影较小,因而耦合效率较低;45°角边入射耦合最大的优点是对探测波长不敏感,但是也仅有51%的光耦合效率;相比之下,光栅耦合可以获得较高的光耦合效率并有利于制备二维探测器阵列,但是制备工艺较为复杂[11,59]。此外,还可采用光学微腔设计、以及光学天线设计来进一步提高光子的吸收效率[6,110]
2015年,普林斯顿大学的Ravikumar等人基于II-VI族ZnCdSe/ZnCdMgSe材料体系,研制了具有4.8 μm和5.8 μm两个中心吸收波长的交错双吸收有源区设计的QCD,获得了从3.3 μm到6 μm宽的光电流谱[105]。2017年,维也纳技术大学的Schwarz等人采用了一个端面耦合低损耗介质脊波导光吸收构型,研制出了具有4.1 μm探测波长的单级联周期QCD,其在温度为300 K时可实现25%的外量子效率,通过进一步优化能带结构来抑制不需要的散射弛豫途径,室温下可获得10 pW/的低噪声等效功率和7×107 cm·Hz1/2·W-1的比探测率[40]。2022年,法国III-V族联合实验室的Quinchard等人报道了一个探测波长在10.3 μm的天线增强的高响应速度QCD,如图12所示,其核心是将有源核嵌入到金属-金属贴片天线中形成8×8的贴片天线谐振器阵列,并与共面波导结构进行单片集成形成天线增强探测器,在温度为295 K时可实现85 mA/W的响应率,室温下的截止频率高达25 GHz[21]。由于天线效应,上述结构可以获得比探测器的电表面大许多的光子收集区域。此外,由于满足子带极化选择规则,该结构允许在正入射下进行有效吸收,从而显著提高信噪比。国内在QCD研究方面取得了一定的研究成果,可实现宽波段响应、较高的响应率和探测率[11,112-114]
QCL和QCD均是基于子带跃迁和共振隧穿的量子级联技术,二者在原理、设计、外延材料以及工艺等方面上较为类似或相同,因此,可以将光源功能和探测功能整合到同一单芯片上,实现单芯片光子集成,可应用于传感和成像等领域[6,115-120]。相比于传统分立元器件的片上功能集成,单芯片光子集成可以大幅减小器件尺寸、减少元器件数量,实现多功能化及小型化。基于同样的外延结构设计和材料,QCL和QCD的功能可以集成到同一个外延片的有源层上,通过改变外加偏压大小来实现激射光源和吸收探测功能的切换[115,116]。然而,QCL和QCD的单芯片集成较为复杂,因为需要同时考虑激光和探测的结构设计因素,包括有源层能带设计、波导设计、光耦合设计以及散热设计等。上述因素中,最大的难点是要对有源层的能带进行精确设计以实现激光发射波长和探测光响应波长的交叠匹配。除此之外,当工作在激光模式下时,上能级应该对电子具有较好的限制作用,而下能级应该对电子具有较好的抽空效果;与之相反,当工作在探测模式下时,上能级应该对电子具有较好的抽空效果,而下能级应该对电子具有较好的限制作用[115,116]。在光耦合方面,QCL激光输出端面应具有较高的外部耦合效率来注入到表面波导,并进一步有效地光耦合到QCD接受端面[6]
QCL和QCD集成器件在2012年由奥地利维也纳技术大学的Schwarz等人首次报道[115],具有双功能有源区的量子级联器件可以在同一个频率/波长下实现激射和探测,该集成QCL和QCD的器件中的双功能有源区在激射和探测模式下的能带图如图13(a)所示,通过外加偏压的切换来分别实现激射和探测功能,在室温下可实现45 mW的脉冲峰值输出功率和3.6 mA/W的响应率,激光和探测谱交叠在6.4 μm到6.8 μm波段[115]。2015年,该研究组通过优化双功能有源区结构,在室温下进一步获得了0.47 W的脉冲输出功率和40 mA/W的响应率,激光和探测波长交叠在6.8 μm附近[116]。2017年,奥地利维也纳技术大学联合美国麻省理工学院和哈佛大学共同研制了8 μm波长的高性能QCL和QCD集成器件,该单管芯集成器件首次可在室温连续工作,连续输出功率高达1 W,响应率为20 mA/W[120]。基于QCL和QCD集成器件以及中红外吸收光谱技术,Schwarz等人进一步研制出了单芯片光子集成传感系统如图13(b)所示,可用于液体和气体的测试,检测精度可达10-6量级[118,119]
量子级联技术的飞速发展加速了产品化进程。中远红外QCL产品类型包括法布里-珀罗FP-QCL、高功率QCL、高峰值功率QCL、宽增益BG-QCL、外腔宽调谐EC-QCL以及分布反馈DFB-QCL等。商业高功率QCL在中波红外(4~5 μm)下的室温连续输出功率超过4 W[22],在长波红外(8~12 μm)下的室温连续输出功率超过2 W[22],在中红外下的脉冲峰值功率可达30 W,而在中红外下的合束输出功率可达15 W[23];商业宽调谐QCL的调谐波数超过300 cm-1[24]。太赫兹QCL产品的激射频率范围在1.8~5 THz,平均输出功率最高达20 mW,可实现脉冲、连续、多模、单模,以及超宽谱(单芯片器件1.6~4.3 THz)等工作模式。由于激光芯片无法单独在室温下工作,太赫兹QCL产品必须配备制冷装置。相比于多元化、高性能的QCL产品,QCD的商业化产品较少。2021年,日本滨松光子学公司发布了全球首款QCD产品,该产品无需制冷和偏压,可以在室温下工作,响应波长为4.65 μm,感光响应率为1 mA/W,截至频率为20 GHz。
由于QCL产品更为成熟,因此,基于QCL的应用研究更为广泛,且在多个领域已逐渐步入实用阶段。在医疗诊断方面,采用QCL成功开展了用于筛查肺癌等疾病的人体呼吸气体检测和血糖检测实验,提供了一种无创疾病筛查新方法[8,12,121]。同时,基于QCL搭建了光纤束传像实验系统,可实现高对比度内窥成像,用于医学诊断和治疗[122]。此外,基于太赫兹QCL开展了生物医学成像研究,用于快速无损诊断[123]。在环境检测方面,基于QCL的红外吸收光谱仪已成功开展对室外大气环境、土壤呼吸气体、汽车尾气等场景气体的检测,检测气体包括各种碳氧化物和氮氧化物等,取得了较高精度的测试结果,探测灵敏度可达10-9量级,且响应速度较快[12,42,124]。在自由空间激光通讯领域,国外的研究人员已采用QCL顺利进行了自由空间激光通信方面的试验探索,证实了QCL可实现远距离红外激光通信的可行性[12]。在2022年,法国的巴黎理工学院等联合研究团队基于直接调制的激射波长为4 μm中波红外QCL进行了自由空间激光通信试验研究,验证了长距离高速传输能力,传输速率可达680 Mbits/s[26]。在红外对抗方面,美国和日本等国家已经加大对基于QCL的新型定向红外对抗系统的研制投入[23,25,41]。2012年,美国诺思罗普·格鲁曼(Northrop Grumman)公司和Daylight Solutions公司得到美国军方的经济支持,共同研发基于QCL的第五代红外对抗系统。目前,采用多波段合束技术可实现高达20 W的输出功率,已成功应用在红外对抗系统并列装于无人机、武装直升机等飞行器中[41]。在遥感探测方面,2016年,美国国家航空航天局(NASA)开启了大气环境层析扫描检测任务(ATOM),利用飞机搭载的QCL红外光谱检测设备来对大气气体进行测量,包括CO2、CO、CH4和N2O等气体,通过改变飞机的高度(0.2~12 km)实现大气气体轮廓扫描诊断[125]。与此同时,NASA还发起了大气碳传输(ACT)任务,基于机载的QCL红外光谱仪来对大气温室气体进行诊断测量,以探寻CO2、CH4等温室气体的来源、传输以及沉降机制[126,127]。在天体观测方面,2014年,美国NASA和德国航空中心共同合作开展平流层红外天文观测台(SOFIA)任务,利用飞机搭载的天文观测设备对火星表面远红外波段的大气进行光谱观测,在观测设备中包含了基于太赫兹QCL的远红外高频通道外差光谱仪,随后在2015年首次观测到了63 μm的原子氧线,用以揭示恒星的形成以及火星大气的演变过程[128,129]。2021年,美国NASA又开启了银河/银河系外超长航时气球光谱太赫兹天文台(GUSTO)任务,利用气球携带具有C、O和N元素发射线探测器的望远镜,该观测设备中同样使用了太赫兹QCL作为局部振荡器,以进一步研究星际间的气体元素(C、O、N),探索星间气体的生命周期以及星云的形成和毁坏过程[129-131]
量子级联技术既可以产生红外到太赫兹波段的激光光源,又可以探测红外到太赫兹波段的电磁波信号,是量子光源和探测领域的重大前沿技术方向,在民用和军用领域具有重要的意义和应用价值。本文首先简要介绍了量子级联技术的原理和发展历史,随后阐述了量子级联器件子带能级结构和电子输运动力学计算思路,接着重点综述了中远红外高功率QCL、中远红外宽调谐QCL、太赫兹QCL、高性能QCD以及QCL和QCD的单芯片光子集成这五方面的国内外技术发展现状,最后介绍了QCL和QCD的产品与应用情况。经过最近三十年的研究,量子级联技术已经在实验室内取得了多次重大突破,已形成多元化和高性能的QCL和QCD商业化产品,并已逐步应用于各类民用和军用领域。量子级联技术的重大成功归因于有源层设计、波导设计、光耦合设计、器件结构优化、外延工艺等关键技术的发展和突破。中红外QCL技术最为成熟,后续应研发大晶圆尺寸的MOCVD(金属有机化合物化学气相沉积)或MOVPE(金属有机化合物气相外延)关键外延技术以降低中红外QCL的成本,从而更好地拓展应用市场。太赫兹QCL目前已可以在261 K的温度下时工作,通过进一步改进有源区和光波导结构设计,相信未来也可以在室温连续波下工作。QCD的研究和应用进展较为缓慢,后续需要进一步优化能带结构并提高光耦合效率来改善室温下的探测性能。QCL和QCD的结合为单芯片光子集成提供了一种解决方案,集成小型化的优势使其可以更好地应用于探测和传感领域,以及应用在侦查、制导、激光武器等国防领域。量子级联技术引领了光源和探测领域的革命,随着技术水平的不断提升,相信在不远的将来,量子级联产品将会更广泛地应用在民用和军用领域并发挥出重要的作用。
  • 国家科技重大专项(J2019-V-0015-0110)
  • 航天科技集团有限公司青年拔尖项目
  • 某部型谱项目(20006873)
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doi: 10.12347/j.ycyk.20231024001
  • 接收时间:2023-10-24
  • 首发时间:2026-03-18
  • 出版时间:2024-05-15
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  • 收稿日期:2023-10-24
  • 修回日期:2024-03-17
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航天科技集团有限公司青年拔尖项目
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    1北京遥测技术研究所 北京 100076
    2大连理工大学集成电路学院 大连 116024
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鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
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