铁电/AlGaN/GaN半导体异质薄膜的界面表征研究
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摘要
界面是功能氧化物/半导体异质薄膜研究的重要内容。功能氧化物/半导体薄膜既具有以半导体载流子的场效应与输运性质,又具有氧化物材料丰富的功能效应,如超导、铁磁、铁电、压电、电光等。如何在功能氧化物/半导体异质界面上,将半导体的场效应与氧化物的功能效应相互集成,诱导出新现象和新效应,进而研制新型器件是当前材料和器件研究的热点之一。尽管功能氧化物/半导体异质薄膜的制备技术在近几年出现了显著的进步,但是,由于理论和实验手段的制约,尤其是界面表征手段的缺乏,人们对功能氧化物/半导体界面有关物理性质和机制的认识还相当有限,阻碍了功能氧化物/半导体异质薄膜及其器件的进一步发展。
本论文以典型的功能氧化物/半导体薄膜——铁电/AlGaN/GaN异质薄膜的界面为主要研究对象,针对三种界面:AlGaN/GaN异质界面、铁电/半导体异质界面和铁电畴壁界面,分别研究界面二维电子气(2DEG)、界面电荷陷阱态、极化反转与畴壁界面运动的表征方法。并以此为基础,研究这些界面特性与铁电/AlGaN/GaN半导体异质薄膜电性能之间的关系。
首先,在纳米尺度上对AlGaN/GaN异质界面2DEG进行了表征研究。采用极弱电容信号的锁相放大技术,研制了微区电容测试系统,局域电容的分辨率达到10 aF(10-18 F)。通过有限元计算模拟,分析了探针针尖与界面2DEG电容与杂散电容的分布规律,发现降低杂散电容和控制针尖接触半径是准确检测局域2DEG电容—电压(C-V)特性的关键。提出“探针电流—半径比例法”,实现了界面局域2DEG浓度的定量检测,测量结果与宏观C-V测试结果具有可比性。利用该方法,发现2 nm超薄介质缓冲层对AlGaN/GaN异质界面2DEG的C-V特性的影响起着决定性的作用。实验结果表明,保证兼容性外延生长的条件下,MgO缓冲层比TiO2缓冲层更利于保持AlGaN/GaN异质界面2DEG的原有特性。
其次,研究了界面电荷陷阱的表征以及电荷陷阱对铁电/AlGaN/GaN异质薄膜电性能的影响。通过建立“铁电/AlGaN”和“AlGaN/GaN”界面陷阱态的等效电导模型,实现了铁电/AlGaN/GaN异质薄膜界面电荷陷阱的定量表征。针对铌酸锂型和钙钛矿型两类典型的铁电/AlGaN/GaN异质薄膜,系统研究了铁电层结构、缓冲层材料、复合缓冲层结构等对界面电荷陷阱密度和分布的影响。研究发现LiNbO3/AlGaN/GaN异质薄膜中存在界面陷阱态和体陷阱态。两种陷阱态具有不同的时间常数,其中,界面陷阱态是影响二维电子气C-V回滞特性的主导因素,而体陷阱态是决定异质薄膜漏电机制的主要原因。与铌酸锂型结构相比,钙钛矿型铁电/AlGaN/GaN结构的界面陷阱态密度较之高出一到两个数量级。采用TiO2/MgO复合缓冲层,可以将无缓冲层的PZT/AlGaN/GaN界面陷阱密度降低一个数量级,达到1011cm-2eV-1,同时显著改善异质结器件的漏电特性。通过降低界面陷阱态和注入电荷,减小了界面电荷对铁电极化的屏蔽作用,改善了铁电极化反转对2DEG的调制作用。
最后,对铁电极化反转特性和电畴的运动特性进行了表征研究。通过建立电极式PFM表征方法,实现了反转过程中电畴演变的监测和局域压电响应回线的测量,解决了宏观极化电滞回线测量无法表征铁电/半导体结构的问题。采用这种方法,对比研究了STO基和GaN基铁电薄膜极化反转过程中畴壁界面运动特性。发现PZT/SrRuO3/TiO2/GaN外延薄膜的极化反转以微区(约1μm)到微区的“成核—融合”方式进行,而且不同微区间新畴的成核特征时间和畴壁的运动速度呈弥散分布。这为解释GaN基铁电薄膜极化反转不同于STO基铁电薄膜的经典成核限制反转机制提供了直接的实验证据,为进一步研究铁电/AlGaN/GaN异质薄膜的极化过程提供了一种新的方法。
Interface is of importance for the functional oxide/semiconductor heterostructured films. The heterostructured films has not only the field effect and the transport properties of charge carriers, but also the fruitful properties of oxides, such as superconducting, ferromagnetic, ferroelectric, piezoelectric, and optioelectic functions. One of the current research focuses is to combine these versatile properties with field effect at the interface. This may induce new phenomena and new effects. Recent years have evident a great advance of the growth method for the function oxide/semiconductor hetero-structured films. However, the further development of the function oxide/semiconductor films is hindered by the limited understanding of their interface properties, especially the lack of efficient characterization methods.
Therefore, in this thesis we focus on the characterization study of the interfaces of ferroelectric/AlGaN/GaN heterostructured thin films, including AlGaN/GaN, ferroelectric/semiconductor (F/S), and ferroelectric domain wall (DW) interfaces. The nanoscale characterization of the two-dimensional electron gas (2DEG) at AlGaN/GaN interfaces, quantitative evaluation of interface trap states at F/S interfaces, and the kinetics of DW interfaces are systematically studied to understand the relationship between macroscopic properties of ferroelectric/AlGaN/GaN and these interface.
For AlGaN/GaN interfaces, the nanoscale characterization of the 2DEG are successfully demonstrated by the home-build nanoscale capacitance spectroscopy (NCS) based on the probe of an atomic force microscopy. The capacitance resolution of NCS is about 10 aF (10x10-18 F). A current measuring method is proposed to determine the contact radius of the probe, and helps our NCS quantitatively characterize the local density of 2DEG. By using NCS, the effect of ultra-thin (~ 2 nm) MgO and TiO2 buffers on the properties of 2DEG is studied. It is found that MgO is superior to TiO2 for preserving the original properties of 2DEG when dielectric oxides are epitaxially grown on the AlGaN/GaN heterostructures.
For F/S interfaces, the trap states are studied by the conductance method. A model for the effective conductance are proposed to separate the contributions of the trap states at the AlGaN/GaN interace and the ferroelectric/AlGaN interface. Using this model, two different trap states, including interface traps and bulk traps are found in the LiNbO3/AlGaN/GaN structure, and the effect of buffers of PZT/AlGaN/GaN on the interface trap density are systematically studied. It is found that LiNbO3/AlGaN/GaN has lower trap densities, and TiO2/MgO buffers are good candidates for reducing taps densities and leakage currents.
In order to characterize the nanoscale DW interfaces and switching processes simultaneously, an electrode-piezoresponse force microscopy (PFM) was developed by combining a PFM with the pulse switching current measurement. Using the electrode-PFM, a comparative study was performed on PZT/SRO/STO, PZT/SRO/TiO2/GaN structures. By imaging the motion of DW interfaces during the polarization switching, a region-by-region nucleation-coalescence process are found in the PZT/SRO/TiO2/GaN structure. This process differs significantly from that of PZT/SRO/STO, which obey classical nucleation-limited-switching model. These characterization methods provide new tools for the further studies of ferroelectric oxide/semiconductor heterostructures.
本论文以典型的功能氧化物/半导体薄膜——铁电/AlGaN/GaN异质薄膜的界面为主要研究对象,针对三种界面:AlGaN/GaN异质界面、铁电/半导体异质界面和铁电畴壁界面,分别研究界面二维电子气(2DEG)、界面电荷陷阱态、极化反转与畴壁界面运动的表征方法。并以此为基础,研究这些界面特性与铁电/AlGaN/GaN半导体异质薄膜电性能之间的关系。
首先,在纳米尺度上对AlGaN/GaN异质界面2DEG进行了表征研究。采用极弱电容信号的锁相放大技术,研制了微区电容测试系统,局域电容的分辨率达到10 aF(10-18 F)。通过有限元计算模拟,分析了探针针尖与界面2DEG电容与杂散电容的分布规律,发现降低杂散电容和控制针尖接触半径是准确检测局域2DEG电容—电压(C-V)特性的关键。提出“探针电流—半径比例法”,实现了界面局域2DEG浓度的定量检测,测量结果与宏观C-V测试结果具有可比性。利用该方法,发现2 nm超薄介质缓冲层对AlGaN/GaN异质界面2DEG的C-V特性的影响起着决定性的作用。实验结果表明,保证兼容性外延生长的条件下,MgO缓冲层比TiO2缓冲层更利于保持AlGaN/GaN异质界面2DEG的原有特性。
其次,研究了界面电荷陷阱的表征以及电荷陷阱对铁电/AlGaN/GaN异质薄膜电性能的影响。通过建立“铁电/AlGaN”和“AlGaN/GaN”界面陷阱态的等效电导模型,实现了铁电/AlGaN/GaN异质薄膜界面电荷陷阱的定量表征。针对铌酸锂型和钙钛矿型两类典型的铁电/AlGaN/GaN异质薄膜,系统研究了铁电层结构、缓冲层材料、复合缓冲层结构等对界面电荷陷阱密度和分布的影响。研究发现LiNbO3/AlGaN/GaN异质薄膜中存在界面陷阱态和体陷阱态。两种陷阱态具有不同的时间常数,其中,界面陷阱态是影响二维电子气C-V回滞特性的主导因素,而体陷阱态是决定异质薄膜漏电机制的主要原因。与铌酸锂型结构相比,钙钛矿型铁电/AlGaN/GaN结构的界面陷阱态密度较之高出一到两个数量级。采用TiO2/MgO复合缓冲层,可以将无缓冲层的PZT/AlGaN/GaN界面陷阱密度降低一个数量级,达到1011cm-2eV-1,同时显著改善异质结器件的漏电特性。通过降低界面陷阱态和注入电荷,减小了界面电荷对铁电极化的屏蔽作用,改善了铁电极化反转对2DEG的调制作用。
最后,对铁电极化反转特性和电畴的运动特性进行了表征研究。通过建立电极式PFM表征方法,实现了反转过程中电畴演变的监测和局域压电响应回线的测量,解决了宏观极化电滞回线测量无法表征铁电/半导体结构的问题。采用这种方法,对比研究了STO基和GaN基铁电薄膜极化反转过程中畴壁界面运动特性。发现PZT/SrRuO3/TiO2/GaN外延薄膜的极化反转以微区(约1μm)到微区的“成核—融合”方式进行,而且不同微区间新畴的成核特征时间和畴壁的运动速度呈弥散分布。这为解释GaN基铁电薄膜极化反转不同于STO基铁电薄膜的经典成核限制反转机制提供了直接的实验证据,为进一步研究铁电/AlGaN/GaN异质薄膜的极化过程提供了一种新的方法。
Interface is of importance for the functional oxide/semiconductor heterostructured films. The heterostructured films has not only the field effect and the transport properties of charge carriers, but also the fruitful properties of oxides, such as superconducting, ferromagnetic, ferroelectric, piezoelectric, and optioelectic functions. One of the current research focuses is to combine these versatile properties with field effect at the interface. This may induce new phenomena and new effects. Recent years have evident a great advance of the growth method for the function oxide/semiconductor hetero-structured films. However, the further development of the function oxide/semiconductor films is hindered by the limited understanding of their interface properties, especially the lack of efficient characterization methods.
Therefore, in this thesis we focus on the characterization study of the interfaces of ferroelectric/AlGaN/GaN heterostructured thin films, including AlGaN/GaN, ferroelectric/semiconductor (F/S), and ferroelectric domain wall (DW) interfaces. The nanoscale characterization of the two-dimensional electron gas (2DEG) at AlGaN/GaN interfaces, quantitative evaluation of interface trap states at F/S interfaces, and the kinetics of DW interfaces are systematically studied to understand the relationship between macroscopic properties of ferroelectric/AlGaN/GaN and these interface.
For AlGaN/GaN interfaces, the nanoscale characterization of the 2DEG are successfully demonstrated by the home-build nanoscale capacitance spectroscopy (NCS) based on the probe of an atomic force microscopy. The capacitance resolution of NCS is about 10 aF (10x10-18 F). A current measuring method is proposed to determine the contact radius of the probe, and helps our NCS quantitatively characterize the local density of 2DEG. By using NCS, the effect of ultra-thin (~ 2 nm) MgO and TiO2 buffers on the properties of 2DEG is studied. It is found that MgO is superior to TiO2 for preserving the original properties of 2DEG when dielectric oxides are epitaxially grown on the AlGaN/GaN heterostructures.
For F/S interfaces, the trap states are studied by the conductance method. A model for the effective conductance are proposed to separate the contributions of the trap states at the AlGaN/GaN interace and the ferroelectric/AlGaN interface. Using this model, two different trap states, including interface traps and bulk traps are found in the LiNbO3/AlGaN/GaN structure, and the effect of buffers of PZT/AlGaN/GaN on the interface trap density are systematically studied. It is found that LiNbO3/AlGaN/GaN has lower trap densities, and TiO2/MgO buffers are good candidates for reducing taps densities and leakage currents.
In order to characterize the nanoscale DW interfaces and switching processes simultaneously, an electrode-piezoresponse force microscopy (PFM) was developed by combining a PFM with the pulse switching current measurement. Using the electrode-PFM, a comparative study was performed on PZT/SRO/STO, PZT/SRO/TiO2/GaN structures. By imaging the motion of DW interfaces during the polarization switching, a region-by-region nucleation-coalescence process are found in the PZT/SRO/TiO2/GaN structure. This process differs significantly from that of PZT/SRO/STO, which obey classical nucleation-limited-switching model. These characterization methods provide new tools for the further studies of ferroelectric oxide/semiconductor heterostructures.
引文
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