ZnO中本征缺陷和掺杂与发光的关系及其作用机理
摘要
ZnO是一种直接带隙的第三代宽禁带半导体,因其在室温下约为3.37 eV的禁带宽度和高达60 meV的激子结合能,而受到了广泛关注,被认为是有望取代GaN的新一代短波长光电子材料。随着ZnO半导体材料制备研究不断取得进展,ZnO基器件特别是光电子器件的研究取得了较大进展。但是ZnO基光电子器件仍未达到实用化水平,其发展遇到了瓶颈,因而需要对ZnO材料的基本问题进行深入研究,如ZnO中的杂质和缺陷,ZnO的生长设备等等。其中ZnO的杂质和缺陷研究尤为重要,因为杂质和缺陷是影响材料性质的重要因素,甚至是决定性因素。
基于这样的背景,本论文着重研究了ZnO中的几种本征缺陷和掺杂与发光的关系,以及它们在ZnO发光中起到的作用。主要工作如下:
首先,创新性地运用Zn扩散掺杂方案,研究了Zn扩散掺杂所形成的缺陷及其对ZnO发光性质的影响。通过对实验结果的分析得出:1)Zn掺杂在ZnO单晶中形成的Zn填隙(Zn_i)缺陷构成离化能约为50 meV的施主,是非故意掺杂ZnO的n型导电的主要来源;2)Zn_i极大地增强了ZnO紫外发光强度,在ZnO的室温紫外发光中起到重要作用。而Zn扩散形成的锌反位缺陷(Zn_o)则对可见光产生贡献:3)在此基础上首次提出自由激子和施主耦合发光的新概念,为分析ZnO室温紫外发光提供了依据。
其次,利用气氛、温度等方法调控缺陷的形成,研究ZnO中各种本征缺陷,如Zn_o、V_o、O_(Zn)等对ZnO可见发光的影响。实验表明,ZnO的可见发光是多种本征缺陷共同作用的结果。通过控制热处理条件(温度和气氛),可以有效改变不同本征缺陷的形成几率,而使ZnO表现出不同的可见发光性质。系统研究ZnO的本征缺陷对于开展ZnO的应用研究具有重要基础作用。
最后,研究Ag掺杂对ZnO光电性质的研究。实验表明,Ag进入ZnO后占据氧位,形成Ag。施主缺陷,在Raman光谱中观察到相应的局域振动模,而且在ZnO禁带中引入新的缺陷能级。
本论文共有6章。
第一章介绍ZnO的晶体结构、基本物理性质、制备方法和应用前景,对固体中的缺陷进行了概述,并提出本论文的工作要点。
第二章利用高压扩散方法研究了Zn扩散掺杂对ZnO单晶中缺陷的影响及其对ZnO单晶紫外发光的影响。结果表明,适合Zn掺杂条件可以使ZnO紫外发光增强近一个数量级,并解释了产生这一现象的原因,并提出了自由激子和锌间隙施主耦合发光的新概念。
第三章研究了ZnO变温PL谱中近带边发射峰峰位随温度变化曲线的规律,重点研究自由激子和Zn间隙施主耦合发光的机理。
第四章利用退火调控方法研究ZnO的本征缺陷发光。结果表明,采用不同的退火条件可以得到不同的本征缺陷,ZnO宽的可见发光峰是多种缺陷共同作用的结果。
第五章研究了Ag掺杂对ZnO光电性质的影响。实验表明Ag掺杂可以在ZnO中引入新的局域振动膜,在ZnO禁带中引入新的缺陷能级。Ag可以占据氧位,形成Ag。施主缺陷。
第六章总结与展望。
ZnO is considered to be the third-generation semiconductor with direct wide-band gap. The semiconductor ZnO has gained substantial interest in the research community in part because of its wide-bind gap(3.37 eV at room temperature) and large exciton binding energy (60 meV) which could lead to prospective applications in shortwave optoelectronics.ZnO is also considered to replace the GaN in the optoelectronics.ZnO based optoelectronic devices make great progress in recent years as a result of the development in the preparation of ZnO materials.However,at present the ZnO based devices have not reached the level of practical use.The development of ZnO meets its bottleneck where the fundamental issues in the ZnO are urgent to be investigated,such as intrinsic defects and impurities in ZnO.Defect and impurities are the dominant factors for the optical or electrical properties of ZnO.So in this dissertation the effects of defects and impurities on the optical and electrical properties of ZnO crystal are investigated.
Considering these research background,the contents of this dissertation are listed as follows:
Firstly,Zn diffusion method was employed to investigate optical and electrical properties resulted from the diffusion of Zn into ZnO crystals.Several important results are obtained:①Zn can diffuse into ZnO crystal and form Zn_i which is a shallow donor with ionization energy of～50 meV.Zn_i is considered as the candidate for residual n-type conductance.②UV emission intensity in ZnO is dramatically enhanced because of Zn_i.In the mean time Zn_o can be formed during Zn diffusing into ZnO and contribute to the visible emission peaked at 2.48 eV.③According to above experimental results,a new emission is proposed to explain the room-temperature UV emission,which is coupling emission of exciton with donor.
Secondly,the effects of intrinsic defect on the visible emission in ZnO crystal are investigated by defect control through ambient and temperature variation.It is suggested that the visible emission in the ZnO is resulted from mutual effect of various intrinsic effects.
Lastly,optical and structural properties of Ag-doped ZnO crystal are studied.It is suggested that Ag diffuse into ZnO and form Ag_o.A local vibrational mode and donor defect level related with Ag_o is observed.
This dissertation is divided into six chapters.
In chapter one,a comprehensive review is given on ZnO in crystal structure, fundamental physical properties,preparation method and prospective applications.
In chapter two,the effects of Zn-doping on the intrinsic defects and ultraviolet emission in ZnO crystal are studied.It is found that the UV emission intensity in room-temperature PL spectra in the Zn-doped ZnO is enhanced by nearly an order compared with the as-grown ZnO.The emission mechanism for this phenomenon is explained.
In chapter three,the temperature dependence of positions of the near-bind-edge emission peaks are investigated.It is found that there are three kinds of temperature dependence which may be resulted from different emission mechanism.A new emission mechanism,coupling emission of excitons with donor,is proposed to explain the UV emission at room temperature.
In chapter four,the annealing control on the intrinsic defects and corresponding photoluminescence is investigated.It is suggested that different annealing condition could lead to different kinds of intrinsic defects and that the visible emission band in ZnO should result from mutual effects of various intrinsic defects.
In chapter five,the Ag is introduced into the ZnO crystal by diffusion method.It is found that a local vibration mode appears in Ag-doped ZnO and that a level is introduced in the gap of ZnO.It is suggested that the Ag atom may diffuse into ZnO crystal and substitute on the oxygen site,forming Ag_o,which is a donor-like defect.
In chapter six,a summary of this dissertation and suggestions for further study.
基于这样的背景,本论文着重研究了ZnO中的几种本征缺陷和掺杂与发光的关系,以及它们在ZnO发光中起到的作用。主要工作如下:
首先,创新性地运用Zn扩散掺杂方案,研究了Zn扩散掺杂所形成的缺陷及其对ZnO发光性质的影响。通过对实验结果的分析得出:1)Zn掺杂在ZnO单晶中形成的Zn填隙(Zn_i)缺陷构成离化能约为50 meV的施主,是非故意掺杂ZnO的n型导电的主要来源;2)Zn_i极大地增强了ZnO紫外发光强度,在ZnO的室温紫外发光中起到重要作用。而Zn扩散形成的锌反位缺陷(Zn_o)则对可见光产生贡献:3)在此基础上首次提出自由激子和施主耦合发光的新概念,为分析ZnO室温紫外发光提供了依据。
其次,利用气氛、温度等方法调控缺陷的形成,研究ZnO中各种本征缺陷,如Zn_o、V_o、O_(Zn)等对ZnO可见发光的影响。实验表明,ZnO的可见发光是多种本征缺陷共同作用的结果。通过控制热处理条件(温度和气氛),可以有效改变不同本征缺陷的形成几率,而使ZnO表现出不同的可见发光性质。系统研究ZnO的本征缺陷对于开展ZnO的应用研究具有重要基础作用。
最后,研究Ag掺杂对ZnO光电性质的研究。实验表明,Ag进入ZnO后占据氧位,形成Ag。施主缺陷,在Raman光谱中观察到相应的局域振动模,而且在ZnO禁带中引入新的缺陷能级。
本论文共有6章。
第一章介绍ZnO的晶体结构、基本物理性质、制备方法和应用前景,对固体中的缺陷进行了概述,并提出本论文的工作要点。
第二章利用高压扩散方法研究了Zn扩散掺杂对ZnO单晶中缺陷的影响及其对ZnO单晶紫外发光的影响。结果表明,适合Zn掺杂条件可以使ZnO紫外发光增强近一个数量级,并解释了产生这一现象的原因,并提出了自由激子和锌间隙施主耦合发光的新概念。
第三章研究了ZnO变温PL谱中近带边发射峰峰位随温度变化曲线的规律,重点研究自由激子和Zn间隙施主耦合发光的机理。
第四章利用退火调控方法研究ZnO的本征缺陷发光。结果表明,采用不同的退火条件可以得到不同的本征缺陷,ZnO宽的可见发光峰是多种缺陷共同作用的结果。
第五章研究了Ag掺杂对ZnO光电性质的影响。实验表明Ag掺杂可以在ZnO中引入新的局域振动膜,在ZnO禁带中引入新的缺陷能级。Ag可以占据氧位,形成Ag。施主缺陷。
第六章总结与展望。
ZnO is considered to be the third-generation semiconductor with direct wide-band gap. The semiconductor ZnO has gained substantial interest in the research community in part because of its wide-bind gap(3.37 eV at room temperature) and large exciton binding energy (60 meV) which could lead to prospective applications in shortwave optoelectronics.ZnO is also considered to replace the GaN in the optoelectronics.ZnO based optoelectronic devices make great progress in recent years as a result of the development in the preparation of ZnO materials.However,at present the ZnO based devices have not reached the level of practical use.The development of ZnO meets its bottleneck where the fundamental issues in the ZnO are urgent to be investigated,such as intrinsic defects and impurities in ZnO.Defect and impurities are the dominant factors for the optical or electrical properties of ZnO.So in this dissertation the effects of defects and impurities on the optical and electrical properties of ZnO crystal are investigated.
Considering these research background,the contents of this dissertation are listed as follows:
Firstly,Zn diffusion method was employed to investigate optical and electrical properties resulted from the diffusion of Zn into ZnO crystals.Several important results are obtained:①Zn can diffuse into ZnO crystal and form Zn_i which is a shallow donor with ionization energy of～50 meV.Zn_i is considered as the candidate for residual n-type conductance.②UV emission intensity in ZnO is dramatically enhanced because of Zn_i.In the mean time Zn_o can be formed during Zn diffusing into ZnO and contribute to the visible emission peaked at 2.48 eV.③According to above experimental results,a new emission is proposed to explain the room-temperature UV emission,which is coupling emission of exciton with donor.
Secondly,the effects of intrinsic defect on the visible emission in ZnO crystal are investigated by defect control through ambient and temperature variation.It is suggested that the visible emission in the ZnO is resulted from mutual effect of various intrinsic effects.
Lastly,optical and structural properties of Ag-doped ZnO crystal are studied.It is suggested that Ag diffuse into ZnO and form Ag_o.A local vibrational mode and donor defect level related with Ag_o is observed.
This dissertation is divided into six chapters.
In chapter one,a comprehensive review is given on ZnO in crystal structure, fundamental physical properties,preparation method and prospective applications.
In chapter two,the effects of Zn-doping on the intrinsic defects and ultraviolet emission in ZnO crystal are studied.It is found that the UV emission intensity in room-temperature PL spectra in the Zn-doped ZnO is enhanced by nearly an order compared with the as-grown ZnO.The emission mechanism for this phenomenon is explained.
In chapter three,the temperature dependence of positions of the near-bind-edge emission peaks are investigated.It is found that there are three kinds of temperature dependence which may be resulted from different emission mechanism.A new emission mechanism,coupling emission of excitons with donor,is proposed to explain the UV emission at room temperature.
In chapter four,the annealing control on the intrinsic defects and corresponding photoluminescence is investigated.It is suggested that different annealing condition could lead to different kinds of intrinsic defects and that the visible emission band in ZnO should result from mutual effects of various intrinsic defects.
In chapter five,the Ag is introduced into the ZnO crystal by diffusion method.It is found that a local vibration mode appears in Ag-doped ZnO and that a level is introduced in the gap of ZnO.It is suggested that the Ag atom may diffuse into ZnO crystal and substitute on the oxygen site,forming Ag_o,which is a donor-like defect.
In chapter six,a summary of this dissertation and suggestions for further study.
引文
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