表面等离子体对纳米结构ZnO膜光致发光性能的调制
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摘要
氧化锌(ZnO)是直接带隙宽禁带化合物半导体材料,其禁带宽度为3.37 eV,在室温下拥有60 meV的激子束缚能,具有高的热稳定性和卓越的光学性质,因此,ZnO成为继GaN之后研究的一个新热点。尽管ZnO薄膜的研究在实验和理论方面都取得了可喜的进展,但是表面等离子体对ZnO薄膜发光的调制机制有待于进一步的研究。
在本论文中,用化学气相沉积法在蓝宝石衬底上生长纳米结构ZnO薄膜,在纳米结构ZnO薄膜表面上利用真空直流溅射仪蒸镀Au纳米颗粒。ZnO薄膜晶体结构用X-射线衍射仪(XRD)表征,结果表明制备的ZnO为纤锌矿六角形结构,和沿c轴择向生长特性。
样品的表面形貌和表面粗糙度分别用扫描电子显微镜(SEM)和原子力显微镜(AFM)测定,SEM测定样品的表面形貌,AFM测试确定样品的表面粗糙度。
通过对ZnO薄膜的光致发光(PL)谱的荧光光谱仪测试,发现多数未蒸镀Au的ZnO薄膜PL谱由两个发射峰组成,一个是波长约380 nm的近带边发射,另一个是约500 nm深能级发射。通常,与可见光发射强度相比,紫外发射的强度相对较弱。而蒸镀Au后的ZnO薄膜PL谱也由紫外发射带和可见光发射带组成,但是,它们的发光强度发生了很大变化。在不同温度下制备的ZnO样品蒸镀Au以后的紫外发射强度和未蒸镀Au的相比,紫外发射强度的增强倍数不同。同时,蒸镀Au前后ZnO薄膜的PL谱中的可见光发射得到不同程度的抑制。关于ZnO薄膜的光致发光的显著的改变,物理机制是入射光的电场和Au纳米颗粒表面的电子耦合,在Au和ZnO的界面处产生了表面等离子体,Au纳米颗粒附近的电场可强烈增强,所以,激发源强度的剧增造成激发过程中激发速率的提高。对于缺陷发光的抑制,可以认为借助金纳米颗粒,缺陷态上的电子被转移到导带上,电荷的转移引起导带电子密度的增加,最终造成紫外发射的增强,使缺陷态电子密度的下降导致可见光发射的抑制。
表面蒸镀Au纳米颗粒的ZnO膜的吸收谱用紫外-可见-近红外分光光度计(UV-VIS-NIR spectrophotometer)测试,实验结果显示在可见光区～500 nm处出现强的吸收峰,此吸收峰由Au纳米颗粒的表面等离子体共振吸收所致。用拉曼光谱仪测试了ZnO的拉曼散射,确定分子的振动模式。
Zinc oxide (ZnO) is a compound semiconductor with direct and wide band gap. It has a band gap of 3.37 eV and an exciton binding energy of 60 meV at room temperature, high thermal stability and excellent optical properties. At present, ZnO has become a new hot spot followed GaN. Although the study of ZnO has been made great processes both in the experimental and theoretical aspects, it is necessary to further study the origin of green emission, the improvement of quality of growth of ZnO, and the mechanism of surface plasmon mediated the luminescence of ZnO,
In this thesis, the pure ZnO thin films with different nanostructures deposited on the sapphire substrates were prepared by a chemical vapor deposition method. A vacuum DC sputtering system was used to deposit Au nanaoparticles on the surface of ZnO nanostructured films. The crystalline structure of ZnO was characterized by X-ray diffractometer (XRD). The results show that all as-prepared ZnO thin films are wurtzite hexagonal structure, and have the strongest peak of ZnO (002). It indicated that the as-grown ZnO films have the perfected orientation growth along c axis.
The surface morphologies and roughness of samples were measured by scanning electron microscopy (SEM) and atomic force microscopy (AFM), respectively. The results showed that the surfaces of samples were not smooth by SEM. The roughness of samples was different by AFM ananlysis results.
The photoluminescence (PL) spectra of ZnO thin films were measured by fluorescence spectrometer. The PL spectra of uncoated ZnO thin films consist of two emission peaks. One is the near band edge emission at around 380 nm, and another is deep level emission due to defects. Moreover, the intensity of UV emission is relatively weaker compared with that of visible emission. The PL spectra of Au-coated ZnO thin films prepared at different temperatures also consist of UV emission band and visible emission band. However, the UV emission intensities of Au-coated samples are enhanced compared with that of un-coated samples. The visible emission intensities of samples were suppressed to some constants. In the case of significant changes in PL of ZnO films, we proposed the following physical mechanism. The electric field of the incident light coupled with Au nanoparticle surface electrons, the surface plasmons were created at the interface between ZnO nanosturcutrues and Au nanoparticles. After light illuminated, the electric field near Au nanoparticles was strongly enhanced. Therefore, the dramatic increase of intensity of excitation source resulted in the improvenment of excitation rate in the excitation process. The electrons located at defect states transferred to conduction band by Au nanoparticles. The charge transfer caused the increase in electron density in conduction band. Finally, UV emission from ZnO was enhanced. Meanwhile the decrease in electron density in defect level resulted in the suppression of the visible emission.
The absorption spectra of Au-coated ZnO films were measured by UV-VIS-NIR spectrophotometer. The experimental results showed that a strong absorption peak at ~ 500 nm occurred in visible region. This absorption peak resulted from the surface plasmon resonance of Au nanopariticles. To investigate the vibration modes of ZnO, Raman scattering spectroscopy was used.
在本论文中,用化学气相沉积法在蓝宝石衬底上生长纳米结构ZnO薄膜,在纳米结构ZnO薄膜表面上利用真空直流溅射仪蒸镀Au纳米颗粒。ZnO薄膜晶体结构用X-射线衍射仪(XRD)表征,结果表明制备的ZnO为纤锌矿六角形结构,和沿c轴择向生长特性。
样品的表面形貌和表面粗糙度分别用扫描电子显微镜(SEM)和原子力显微镜(AFM)测定,SEM测定样品的表面形貌,AFM测试确定样品的表面粗糙度。
通过对ZnO薄膜的光致发光(PL)谱的荧光光谱仪测试,发现多数未蒸镀Au的ZnO薄膜PL谱由两个发射峰组成,一个是波长约380 nm的近带边发射,另一个是约500 nm深能级发射。通常,与可见光发射强度相比,紫外发射的强度相对较弱。而蒸镀Au后的ZnO薄膜PL谱也由紫外发射带和可见光发射带组成,但是,它们的发光强度发生了很大变化。在不同温度下制备的ZnO样品蒸镀Au以后的紫外发射强度和未蒸镀Au的相比,紫外发射强度的增强倍数不同。同时,蒸镀Au前后ZnO薄膜的PL谱中的可见光发射得到不同程度的抑制。关于ZnO薄膜的光致发光的显著的改变,物理机制是入射光的电场和Au纳米颗粒表面的电子耦合,在Au和ZnO的界面处产生了表面等离子体,Au纳米颗粒附近的电场可强烈增强,所以,激发源强度的剧增造成激发过程中激发速率的提高。对于缺陷发光的抑制,可以认为借助金纳米颗粒,缺陷态上的电子被转移到导带上,电荷的转移引起导带电子密度的增加,最终造成紫外发射的增强,使缺陷态电子密度的下降导致可见光发射的抑制。
表面蒸镀Au纳米颗粒的ZnO膜的吸收谱用紫外-可见-近红外分光光度计(UV-VIS-NIR spectrophotometer)测试,实验结果显示在可见光区～500 nm处出现强的吸收峰,此吸收峰由Au纳米颗粒的表面等离子体共振吸收所致。用拉曼光谱仪测试了ZnO的拉曼散射,确定分子的振动模式。
Zinc oxide (ZnO) is a compound semiconductor with direct and wide band gap. It has a band gap of 3.37 eV and an exciton binding energy of 60 meV at room temperature, high thermal stability and excellent optical properties. At present, ZnO has become a new hot spot followed GaN. Although the study of ZnO has been made great processes both in the experimental and theoretical aspects, it is necessary to further study the origin of green emission, the improvement of quality of growth of ZnO, and the mechanism of surface plasmon mediated the luminescence of ZnO,
In this thesis, the pure ZnO thin films with different nanostructures deposited on the sapphire substrates were prepared by a chemical vapor deposition method. A vacuum DC sputtering system was used to deposit Au nanaoparticles on the surface of ZnO nanostructured films. The crystalline structure of ZnO was characterized by X-ray diffractometer (XRD). The results show that all as-prepared ZnO thin films are wurtzite hexagonal structure, and have the strongest peak of ZnO (002). It indicated that the as-grown ZnO films have the perfected orientation growth along c axis.
The surface morphologies and roughness of samples were measured by scanning electron microscopy (SEM) and atomic force microscopy (AFM), respectively. The results showed that the surfaces of samples were not smooth by SEM. The roughness of samples was different by AFM ananlysis results.
The photoluminescence (PL) spectra of ZnO thin films were measured by fluorescence spectrometer. The PL spectra of uncoated ZnO thin films consist of two emission peaks. One is the near band edge emission at around 380 nm, and another is deep level emission due to defects. Moreover, the intensity of UV emission is relatively weaker compared with that of visible emission. The PL spectra of Au-coated ZnO thin films prepared at different temperatures also consist of UV emission band and visible emission band. However, the UV emission intensities of Au-coated samples are enhanced compared with that of un-coated samples. The visible emission intensities of samples were suppressed to some constants. In the case of significant changes in PL of ZnO films, we proposed the following physical mechanism. The electric field of the incident light coupled with Au nanoparticle surface electrons, the surface plasmons were created at the interface between ZnO nanosturcutrues and Au nanoparticles. After light illuminated, the electric field near Au nanoparticles was strongly enhanced. Therefore, the dramatic increase of intensity of excitation source resulted in the improvenment of excitation rate in the excitation process. The electrons located at defect states transferred to conduction band by Au nanoparticles. The charge transfer caused the increase in electron density in conduction band. Finally, UV emission from ZnO was enhanced. Meanwhile the decrease in electron density in defect level resulted in the suppression of the visible emission.
The absorption spectra of Au-coated ZnO films were measured by UV-VIS-NIR spectrophotometer. The experimental results showed that a strong absorption peak at ~ 500 nm occurred in visible region. This absorption peak resulted from the surface plasmon resonance of Au nanopariticles. To investigate the vibration modes of ZnO, Raman scattering spectroscopy was used.
引文
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