Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第16857号 / 工博第3578号 / 新制||工||1541(附属図書館) / 29532 / 京都大学大学院工学研究科電子工学専攻 / (主査)教授 野田 進, 教授 川上 養一, 教授 藤田 静雄 / 学位規則第4条第1項該当

abstract: Wurtzite (In, Ga, Al) N semiconductors, especially InGaN material systems, demonstrate immense promises for the high efficiency thin film photovoltaic (PV) applications for future generation. Their unique and intriguing merits include continuously tunable wide band gap from 0.70 eV to 3.4 eV, strong absorption coefficient on the order of ∼105 cm−1, superior radiation resistance under harsh environment, and high saturation velocities and high mobility. Calculation from the detailed balance model also revealed that in multi-junction (MJ) solar cell device, materials with band gaps higher than 2.4 eV are required to achieve PV efficiencies greater than 50%, which is practically and easily feasible for InGaN materials. Other state-of-art modeling on InGaN solar cells also demonstrate great potential for applications of III-nitride solar cells in four-junction solar cell devices as well as in the integration with a non-III-nitride junction in multi-junction devices. This dissertation first theoretically analyzed loss mechanisms and studied the theoretical limit of PV performance of InGaN solar cells with a semi-analytical model. Then three device design strategies are proposed to study and improve PV performance: band polarization engineering, structural design and band engineering. Moreover, three physical mechanisms related to high temperature performance of InGaN solar cells have been thoroughly investigated: thermal reliability issue, enhanced external quantum efficiency (EQE) and conversion efficiency with rising temperatures and carrier dynamics and localization effects inside nonpolar m-plane InGaN quantum wells (QWs) at high temperatures. In the end several future work will also be proposed. Although still in its infancy, past and projected future progress of device design will ultimately achieve this very goal that III-nitride based solar cells will be indispensable for today and future’s society, technologies and society. / Dissertation/Thesis / Doctoral Dissertation Electrical Engineering 2020

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Parmi les nitrures III-V, le matériau InGaN a été intensément étudié depuis les années 2000 pour des applications photovoltaïques, en particulier pour des cellules multi-jonctions, grâce à son large gap modulable pouvant couvrir quasiment tout le spectre solaire. On pourrait alors atteindre de hauts rendements tout en assurant de bas coûts. Cependant, l’un des problèmes de l’InGaN est l’absence de substrat accordé en maille provoquant une grande densité de défauts et limitant ainsi les performances des composants. Nous avons donc étudié la faisabilité de cellules solaires simples jonctions à base d’InGaN sur des substrats alternatifs comme le silicium et le verre afin de baisser les coûts et d’avoir de larges applications. Afin d’adapter l’InGaN sur ces substrats alternatifs, nous avons utilisé une couche tampon en ZnO. Ce travail a été réalisé dans le cadre du projet ANR NewPVonGlass. Plus particulièrement, dans ce projet, mon travail avait pour objectifs de réaliser des caractérisations électriques et optiques des matériaux et des composants. Les deux premières parties de cette thèse introduisent le matériau InGaN et l’effet photovoltaïque. Les techniques de caractérisation utilisées sont expliquées dans le troisième chapitre. Ensuite, les résultats obtenus lors de la caractérisation cristalline du matériau InGaN sont présentés en fonction du substrat, de la concentration d’indium et de l’épaisseur de la couche. Puis, la cinquième partie développe les caractérisations des premières cellules à base d’InGaN sur saphir. Enfin, dans le dernier chapitre, des simulations de cellules solaires à base d’InGaN ont été réalisées. Le modèle développé nous a permis d’optimiser la structure et le dopage du composant et de déterminer les paramètres critiques. Nous montrons donc, dans ce travail, le développement d’une cellule solaire à base d’InGaN : des caractérisations des matériaux de base à celles des cellules solaires, en passant par la modélisation. / Among III-V nitrides, the InGaN material has intensively been studied since the year 2000 for photovoltaic applications, in particular for multi-junction solar cells, thanks to its large tunable band gap covering almost the entire solar spectrum. Then, it will be possible to reach high efficiency and low cost. However, one of the problems of InGaN material is the absence of lattice-matched substrate leading to high defect density which limits device performances. We have thus studied the feasibility of single junction InGaN based solar cells on alternative substrate such as silicon and glass in order to lower the price and to benefit from their wide application fields. To adapt InGaN material on these new substrates, we have utilized ZnO buffer layer. This work has been carried out within the framework of the ANR project NewPVonGlass. More particularly, in this project, I was in charge of the electrical and optical characterizations of the materials and devices. In the two first parts of this manuscript, the InGaN material and the photovoltaic effect are introduced. Then, the characterization techniques are explained in the third chapter. In the fourth part, the results obtained during crystalline characterization of the InGaN materials are presented depending on the substrate, the indium percentage and the InGaN layer thickness. Then, the fifth chapter presents the first InGaN-based solar cell characteristics on sapphire substrate. Finally, in the last part, simulations of InGaN-based solar cell have been performed. The developed model was able to optimize the structure and to determine the critical parameters. Thus, we have shown in this work the development of an InGaN-based solar cell from the base material characterizations to the device tests, through modeling.

The popularity of III-nitride materials has taken up the semiconductor industry to newer applications because of their remarkable properties. In addition to having a direct and wide band gap of 3.4 eV, a very fascinating property of GaN is the band gap tuning from 0.7 to 6.2 eV by alloying with Al or In. The most common orientation to grow optoelectronic devices out of these materials are the polar c-plane which are strongly affected by the intrinsic spontaneous and piezoelectric polarization fields. Devices grown in no polar orientation such as (1 0 –1 0) m-plane or (1 1 –2 0) a-plane have no polarization in the growth direction and are receiving a lot of focus due to enhanced behaviour. The first part of this thesis deals with the development of non-polar epimGaN films of usable quality, on an m-plane sapphire by plasma assisted molecular beam epitaxy. Growth conditions such as growth temperature and Ga/N flux ratio were tuned to obtain a reasonably good crystalline quality film. MSM photodetectors were fabricated from (1 0 -1 0) m-GaN, (1 1 -2 0) a-GaN and semipolar (1 1 -2 2) GaN films and were compared with the polar (0 0 0 2) c-GaN epilayer. Later part of the thesis investigated (1 0 -1 0) InN/ (1 0 -1 0) GaN heterostructures. Further, we could successfully grow single composition nonpolar a-plane InxGa1-xN epilayers on (1 1 -2 0) GaN / (1 -1 0 2) sapphire substrate. This thesis focuses on the growth and characterisation of nonpolar GaN, InxGa1-xN and InN by plasma assisted molecular beam epitaxy and on their photodetection potential. Chapter 1 explains the motivation of this thesis work with an introduction to the III-nitride material and the choice of the substrate made. Polarization effect in the polar, nonpolar and semipolar oriented growth is discussed. Fabrication of semiconductor photodetectors and its principle is explained in details. Chapter 2 discusses the various experimental tools used for the growth and characterisation of the film. Molecular beam epitaxy technique is elaborately explained along with details of the calibration for the BEP of various effusion cells along with growth temperature at the substrate. Chapter 3 discusses the consequence of nitridation on bare m-sapphire substrate. Impact of nitridation step prior to the growth of GaN film over (1 0 -1 0) m-sapphire substrate was also studied. The films grown on the nitridated surface resulted in a nonpolar (1 0 -1 0) orientation while without nitridation caused a semipolar (1 1 -2 2) orientation. Room temperature photoluminescence study showed that nonpolar GaN films have higher value of compressive strain as compared to semipolar GaN films, which was further confirmed by room temperature Raman spectroscopy. The room temperature UV photodetection of both films was investigated by measuring the I-V characteristics under UV light illumination. UV photodetectors fabricated on nonpolar GaN showed better characteristics, including higher external quantum efficiency, compared to photodetectors fabricated on semipolar GaN. Chapter 4 focuses on the optimization and characterisation of nonpolar (1 0 -1 0) m-GaN on m-sapphire by molecular beam epitaxy. A brief introduction to the challenges in growing a pure single phase nonpolar (1 0 -1 0) GaN on (1 0 -1 0) sapphire without any other semipolar GaN growth is followed by our results achieving the same. Effect of the growth temperature and Ga/N ratio on the structural and optical properties of m-GaN epilayers was studied and the best condition was obtained for the growth temperature of 7600C and nitrogen flow of 1 sccm. Strain in the film was quantitatively measured using Raman spectroscopy and qualitatively analyzed by RSM. Au/ nonpolar GaN schottky diode was fabricated and temperature dependent I-V characteristics showed rectifying nature. Chapter 5 demonstrates the growth of (1 0 -1 0) m-InN / (1 0 -1 0) m-GaN / (1 0 -1 0) m-sapphire substrate. Nonpolar InN layer was grown at growth temperature ranging from 3900C to 440C to obtain a good quality film at 4000C. An in-plane relationship was established for the hetrostructures using phi-scan and a perfect alignment was found for the epilayers. RSM images on the asymmetric plane revealed highly strained layers. InN band gap was found to be around 0.8 eV from absorption spectra. The valance band offset value is calculated to be 0.93 eV for nonpolar m-plane InN/GaN heterojunctions. The heterojunctions form in the type-I straddling configuration with a conduction band offsets of 1.82 eV. Chapter 6 focuses on the optimization of nonpolar (1 1 -2 0) a-GaN on (1 -1 0 2) r-sapphire by molecular beam epitaxy. Effect of the growth temperature and Ga/N ratio on the structural and optical properties of a-GaN epilayers was studied and the best condition was obtained for the growth temperature of 7600C and nitrogen flow of 1 sccm. An in-plane orientation relationship is found to be [0 0 0 1] GaN || [-1 1 0 1] sapphire and [-1 1 0 0] GaN || [1 1 -2 0] sapphire for nonpolar GaN on r-sapphire substrate. Strain in the film was quantitatively measured using Raman spectroscopy and qualitatively analyzed by RSM. UV photo response of a-GaN film was measured after fabricating an MSM structure over the film with Au. EQE of the photodetectors fabricated in the (0 0 0 2) polar and (1 1 -2 0) nonpolar growth directions were compared in terms of responsively, nonpolar a-GaN showed the best sensitivity at the cost of comparatively slow response time. Chapter 7 demonstrates the growth of non-polar (1 1 -2 0) a-plane InGaN epilayers on a-plane (1 1 -2 0) GaN/ (1 -1 0 2) r-plane sapphire substrate using PAMBE. The high resolution X-ray diffraction (HRXRD) studies confirmed the orientation of the films and the compositions to be In0.19Ga0.81N, In0.21Ga0.79N and In0.23Ga0.77N. The compositions of the films were controlled by the growth parameters such as growth temperature and indium flux. Effect of variation of Indium composition on the strain of the epilayers was analyzed from the asymmetric RSM images. Further, we report the growth of self-assembled non-polar high indium clusters of In0.55Ga0.45N over non-polar (1 1 -2 0) a-plane In0.17Ga0.83N epilayer grown on a-plane (1 1 -2 0) GaN / (1 -1 0 2) r-plane sapphire substrate. The structure hence grown when investigated for photo-detecting properties, showed sensitivity to both infrared and ultraviolet radiations due to the different composition of InGaN region. Chapter 8 concludes with the summary of present investigations and the scope for future work.

Doctor of Philosophy / Department of Physics / Hongxing Jiang / InGaN based, blue and green light emitting diodes (LEDs) have been successfully produced over the past decade. But the progress of these LEDs is often limited by the fundamental problems of InGaN such as differences in lattice constants, thermal expansion coefficients and physical properties between InN and GaN. This difficulty could be addressed by studying pure InN and In[subscript]xGa[subscript]1-xN alloys. In this context Ga-rich In[subscript]xGa[subscript]1-xN (x≤ 0.4) epilayers were grown by metal organic chemical vapor deposition (MOCVD). X-ray diffraction (XRD) measurements showed In[subscript]xGa[subscript]1-xN films with x= 0.37 had single phase. Phase separation occurred for x ~ 0.4. To understand the issue of phase separation in Ga-rich In[subscript]xGa[subscript]1-xN, studies on growth of pure InN and In-rich In[subscript]xGa[subscript]1-xN alloys were carried out. InN and In-rich In[subscript]xGa[subscript]1-xN (x~0.97- 0.40) epilayers were grown on AlN/Al[subscript]2O[subscript]3 templates. A Hall mobility of 1400 cm[superscript]2/Vs with a carrier concentration of 7x1018cm[superscript]-3 was observed for InN epilayers grown on AlN templates. Photoluminescence (PL)emission spectra revealed a band to band emission peak at ~0.75 eV for InN. This peak shifted to 1.15 eV when In content was varied from 1.0 to 0.63 in In-rich In[subscript]xGa[subscript]1-xN epilayers. After growth parameter optimization of In- rich In[subscript]xGa[subscript]1-xN alloys with (x= 0.97-0.40) were successfully grown without phase separation. Effects of Mg doping on the PL properties of InN epilayers grown on GaN/Al[subscript]2O[subscript]3 templates were investigated. An emission line at ~ 0.76 eV, which was absent in undoped InN epilayers and was about 60 meV below the band edge emission peak at ~ 0.82 eV, was observed to be the dominant emission in Mg-doped InN epilayers. PL peak position and the temperature dependent emission intensity corroborated each other and suggested that Mg acceptor level in InN is about 60 meV above the valance band maximum. Strain effects on the emission properties of InGaN/GaN multiple quantum wells (MQWs) were studied using a single blue LED wafer possessing a continuous variation in compressive strain. EL emission peak position of LEDs varies linearly with the biaxial strain; a coefficient of 19 meV/GPa, characterizes the relationship between the band gap energy and biaxial stress of In[subscript]0.2Ga[subscript]0.8N/GaN MQWs.

InGaN based blue and near-ultraviolet light emitting diodes and laser diodes have been successfully commercialized for many applications such as general lighting, display backlighting and high density optical storage devices. Despite having a comparably high defect density, these devices are known for their efficient operation, which is attributed to localization in potential fluctuations preventing carriers from reaching the centers of nonradiative recombination. Nitride research is currently headed towards improving deep ultraviolet AlGaN and green InGaN emitters with higher Al and In molar fractions. The efficiency of these devices trails behind the blue counterparts as the carrier localization does not seem to aid in supressing nonradiative losses. In addition, the operation of ternary nitride heterostructure based devices is further complicated by the presence of large built-in electric fields. Although the problem can be ameliorated by growing structures in nonpolar or semipolar directions, the step from research to production still awaits. In this thesis, carrier dynamics and localization effects have been studied in three different nitride ternary compounds: AlGaN epitaxial layers and quantum wells with high Al content, nonpolar m-plane InGaN/GaN quantum wells and lattice matched AlInN/GaN heterostructures. The experimental methods of this work mainly consist of spectroscopy techniques such as time-resolved photoluminescence and differential transmission pump-probe measurements as well as spatial photoluminescence mapping by means of scanning near-field microscopy. The comparison of luminescence and differential transmission measurements has allowed estimating the localization depth in AlGaN quantum wells. Additionally, it has been demonstrated that the polarization degree of luminescence from m-InGaN quantum wells decreases as carriers diffuse to localization centers.What is more, dual-scale localization potential has been evidenced by near-field measurements in both AlGaN and m-InGaN. Larger scale potential fluctuation have been observed directly and the depth of nanoscopic localization has been estimated theoretically from the recorded linewidth of the near-field spectra. Lastly, efficient carrier transport has been observed through AlInN layer despite large alloy inhomogeneities evidenced by broad luminescence spectra and the huge Stokes shift. Inhomogeneous luminescence from the underlying GaN layer has been linked to the fluctuations of the built-in electric field at the AlInN/GaN interface. / <p>QC 20121101</p>

With rapid development of light emitting device, the detection techniques of semiconductor are more and more important, which include time-resolved photoluminescence (TRPL) and optical beam induced current (OBIC) microscopy. In this thesis, we realize the carrier behaviors of active region with multiple quantum wells (MQWs) by these microscopies, and the samples are light emitting diodes (LEDs). However, PL intensity of LEDs increase but OBIC not due to external field compensates, on the other hand, reducing PL lifetime indicates the response time of device shorter with higher reverse bias.

Ce travail a porté sur la croissance par épitaxie par jets moléculaires de nanofils InGaN/GaNsur Si (111).Le dépôt d'InGaN en conditions riches azote sur des nanofi ls GaN pré-existants permet deconserver la structure colonnaire. La morphologie des nanofi ls s'est révélée dépendre fortementdu taux d'indium utilisé dans les fl ux. A faible taux nominal d'indium celui-ci se concentre dansle coeur du fi l, ce qui résulte en une structure coeur-coquille InGaN-GaN spontanée. Malgré letaux d'indium important dans le coeur, la relaxation des contraintes y est entièrement élastique.La luminescence est dominée par des eff ets de localisation de porteurs qui donnent lieu à unebonne tenue en température. Au contraire, à plus fort flux nominal d'indium il y a relaxationplastique des contraintes et aucune séparation de phase n'est observée.L'étude d'insertions InGaN permet de con firmer que, malgré le faible diamètre des nano fils, lacroissance est dominée par la nécessité de relaxation des contraintes, et la nucléation de l'InGaNse fait sous la forme d'un îlot facetté. Il en résulte une incorporation préférentielle de l'indiumau sommet de l'îlot, et donc un gradient radial de composition qui se développe en structurecoeur-coquille spontanée au cours de la croissance.Au contraire, la croissance en conditions riches métal entraîne une croissance latérale trèsimportante, nettement plus marquée dans le cas d'InGaN que de GaN : l'indium en excès a une ffet surfactant qui limite la croissance axiale et favorise la croissance latérale.