铝掺杂量对氧化锌薄膜光电性能的影响
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摘要
近年来,由于Al掺杂ZnO薄膜(ZnO:Al)具有优良的光电性能,又因其原料丰富、成本低廉以及在氢等离子体环境中稳定等优点,已经成为透明导电薄膜领域的研究和应用热点之一。
ZnO:Al薄膜通常作为透明电极材料广泛地应用于光伏器件和OLED器件中。低电阻率和可见光区高透过率是影响电极材料的两个重要因素。为了降低薄膜电阻率,通常把Al原子掺入到ZnO晶格中成为替位原子,从而增加晶格中自由载流子浓度,提高薄膜的导电性。如果Al掺杂量过低,薄膜导电性得不到提高；如果Al掺杂量过高,过剩的Al原子不但会成为晶格缺陷降低载流子浓度和迁移率,而且还会成为晶格散射中心降低薄膜在可见光区的透光率。所以只有在适量铝掺杂范围内,才能使薄膜兼具优良的光学和电学性能。因此,探究Al掺杂量对ZnO:Al薄膜光电性能的影响有一定的实际意义。
本文分别采用Al掺杂含量为1wt.%、2wt.%、3wt.%的Zn/Al合金靶材和Al掺杂含量为2wt.%的A1203陶瓷靶材,利用直流磁控溅射技术在玻璃衬底上制备了ZnO:Al薄膜。利用扫描电子显微镜(SEM)、PANalytical XRD衍射系统(XRD)、传统四探针、UV-3150型IR-VIS-UV分光光度计、HMS-3000Hall测试仪分别研究掺杂含量和各种工艺参数对ZnO:Al薄膜的结构、电学(载流子浓度、迁移率和电阻率)和光学特性的影响,研究结果如下：
(1)研究不同Al掺杂量ZnO:Al薄膜电学性能受衬底温度的影响。实验得出：随着掺杂量的增加(1～3wt%),反应最佳衬底温度值减小,分别在230℃、210℃、180℃时对应电阻率最低,分别为6.3×10-4Ω·cm、7×10-4Ω·cm和1×10-3Ω·cm.我们从溅射气相原子与衬底间能量交换行为的角度分析。
(2)选取Al掺杂量不同的ZnO:Al薄膜样品(电阻率相同),研究掺杂量对薄膜光学的性能。实验得出：在紫外波段,随着掺杂浓度的增加,吸收限发生“蓝移”。在近红外波段(800-1100nm)1wt.%的ZnO:Al透光率明显高于2wt.%、3wt.%的ZnO:Al薄膜。这主要是因为1wt.% ZnO:Al的载流子浓度低,自由载流子对光子的吸收少引起的。
(3)选取Al掺杂量不同的ZnO:Al薄膜样品(电阻率相同),利用Hall效应测试探究铝掺杂量对薄膜载流子浓度和载流子迁移率的影响。实验得出：在三个样品电阻率大致相同的情况下,随着掺杂量的增加,薄膜的载流子浓度逐渐增加,但薄膜载流子的迁移率逐渐下降。我们从掺杂机制和迁移率的散射机制方面给予解释。
(4)采用2wt.%Al掺杂的陶瓷靶材制备ZnO:Al薄膜,研究氧气流量和衬底温度对薄膜光电性能的影响,同时与2wt.%Al掺杂的合金靶材制备的ZnO:Al薄膜比较衬底温度对它们电阻率的影响。实验得出：①薄膜电阻率随着氧气流量的增加急剧增大。当氧气流量为0.22sccm时,薄膜电阻率最小为5.02×104/Ω·cm,载流子浓度为4.237×1020/cm-3,迁移率29.32cm2/V·s。②薄膜电阻率随着衬底温度的升高逐渐降低。当衬底温度为400℃时,电阻率达到最低4.7×10-4Ω·cm.③与2wt.%Al掺杂的合金靶材制备的ZnO:Al薄膜比较得出：合金靶材制备的ZnO:Al薄膜所需衬底温度较低,当在210℃时,电阻率达到最低最低6.74×10-4Ω·cm.我们从合金靶材反应溅射和陶瓷靶材的溅射机理方面给予解释。
(5)系统研究了1wt.%Al掺杂的ZnO:Al薄膜电阻率受衬底温度的影响,并且将其作为阳极应用到OLED器件中。实验得出：①当衬底温度为230℃时,电阻率最小,阻值为6×10-4Ω·cm。②与相同电阻率的ITO阳极制备的OLED器件对比看出,两种器件都表现出典型的二极管特性。但是从电流密度、发光亮度和电流效率三方面角度来看,AZO薄膜阳极器件均低于ITO薄膜阳极器件的性能。初步分析原因是AZO薄膜的功函数略小于ITO薄膜的功函数,导致阳极空穴注入能力相对降低。
Recently,Al doped ZnO film (ZnO:Al) is a promising transparent conductive film because of its satisfactory electrical and optical properties, low cost of raw materials and stability in hydrogen plasma environment.
ZnO:Al thin film as electrode materials commonly used in photovoltaic devices and OLED devices. Low resistivity and high visible light transmittance are two important factors which can impact on electrode materials. In order to reduce the film resistivity, usually make an appropriate amount of aluminum ions into the ZnO lattice. Aluminum doping content increases concentration of crystal free carrier, thereby enhancing the conductivity properties of ZnO thin films. If the Al doping level is low, the film conductivity can not increase; if Al doping is too high, the excess Al atoms into the lattice not only reduce the carrier concentration and mobility, but also as a lattice scattering Center lower film transmittance in visible region. Can be seen only in the amount of aluminum doping range, can the film both excellent optical and electrical properties. Therefore, the inquiry on Al doped ZnO:Al thin film optical properties is particularly important.
In this paper, the transparent and conductive AZO films were deposited on glass substrate by DC reactive magnetron sputtering from Zn/Al alloy targets doped with 1,2 and 3wt.%and ZnO/Al2O3 ceramic target doped with 2wt.% Al2O3, respectively. The effect of deposition parameters on the structural, electrical and optical properties of AZO films was investigated systematically by scanning electron microscopy (SEM), PANalytical x-ray diffractometry (XRD), four point probe,UV-VIS-IR spectrophotometry and HMS-3000 Hall effect measurement system,respectively. The results indicate:
(1) Effect of substrate temperature on the electrical properties of ZnO:Al thin films with different Al-doped content was investigated. The results showed that with the increasing dopant content the substrate's optimum reaction temperture lowers,at 230℃,210℃,180℃when the resistivity corresponds to a minimum. Respectively, 6.3×10-4Ω·cm、7×10-4Ω·cm and 1×10-3Ω·cm.
(2) Select the same resistivity of ZnO.Al thin film samples with different Al-doped content to study the optical properties. The results showed that in the UV band the blue shifts of the optical absorption edge occurred with the increasing doping concentration. Moreover, in the near-infrared band (800-1100nm) 1wt.% transmittance of AZO was significantly higher than 2,3wt.% of the films. This is mainly because high carrier concentration produces undesirable infrared (IR) absorption by free carriers.
(3) Select the same resistivity of ZnO:Al thin film samples with different Al-doped content to study the electrical properties include carrier concentration and carrier mobility rate by HMS-3000 Hall effect measurement system. The results showed that as the doping increases, the film carrier concentration gradually increased, but the film carrier mobility rate gradually decreased. We mixed scattering mechanism and the mobility of mechanisms to give an explanation.
(4) With 2wt.% Al-doped ceramic target preparation of ZnO:Al thin films to study the substrate temperature on the thin film photovoltaic performance. The results showed that with the substrate temperature increasing, the film resistivity decreased gradually. When the substrate temperature is 390℃, the resistance reached the lowest rate of 4.7×10-4Ω·cm. Then with 2wt.% Al alloy target prepared doped ZnO:Al thin-film comparison of temperature on the resistivity of their impact. The results showed that the ceramic target of the AZO thin films prepared by different alloy target prepared AZO films when the substrate temperature is 210℃, the lowest resistivity of up to 6.74×10-4Ω·cm. Once the deviation from this temperature resistivity of the will increase. We are from the alloy target by reactive sputtering, and ceramic target in the sputtering mechanism to give an explanation.
(5) Systematic study of substrate temperature on lwt.% ZnO:Al thin film resistivityobtained when the substrate temperature of 230℃, the resistivity minimum, resistance to 6×10-4Ω·cm. Then, this sample as an anode applied to the OLED device, and with the same resistivity of the ITO anode prepared by the efficiency of OLED devices for comparison. The results showed that both devices showed typical diode characteristics. However, from the current density, luminance and current efficiency point of view of three aspects, AZO thin film devices are less than the ITO thin film anode anode device performance. The reason is a preliminary analysis of the work function of AZO thin films slightly less than the work function of ITO thin films, leading to the anode hole injection capacity and relatively cheap.
ZnO:Al薄膜通常作为透明电极材料广泛地应用于光伏器件和OLED器件中。低电阻率和可见光区高透过率是影响电极材料的两个重要因素。为了降低薄膜电阻率,通常把Al原子掺入到ZnO晶格中成为替位原子,从而增加晶格中自由载流子浓度,提高薄膜的导电性。如果Al掺杂量过低,薄膜导电性得不到提高；如果Al掺杂量过高,过剩的Al原子不但会成为晶格缺陷降低载流子浓度和迁移率,而且还会成为晶格散射中心降低薄膜在可见光区的透光率。所以只有在适量铝掺杂范围内,才能使薄膜兼具优良的光学和电学性能。因此,探究Al掺杂量对ZnO:Al薄膜光电性能的影响有一定的实际意义。
本文分别采用Al掺杂含量为1wt.%、2wt.%、3wt.%的Zn/Al合金靶材和Al掺杂含量为2wt.%的A1203陶瓷靶材,利用直流磁控溅射技术在玻璃衬底上制备了ZnO:Al薄膜。利用扫描电子显微镜(SEM)、PANalytical XRD衍射系统(XRD)、传统四探针、UV-3150型IR-VIS-UV分光光度计、HMS-3000Hall测试仪分别研究掺杂含量和各种工艺参数对ZnO:Al薄膜的结构、电学(载流子浓度、迁移率和电阻率)和光学特性的影响,研究结果如下：
(1)研究不同Al掺杂量ZnO:Al薄膜电学性能受衬底温度的影响。实验得出：随着掺杂量的增加(1～3wt%),反应最佳衬底温度值减小,分别在230℃、210℃、180℃时对应电阻率最低,分别为6.3×10-4Ω·cm、7×10-4Ω·cm和1×10-3Ω·cm.我们从溅射气相原子与衬底间能量交换行为的角度分析。
(2)选取Al掺杂量不同的ZnO:Al薄膜样品(电阻率相同),研究掺杂量对薄膜光学的性能。实验得出：在紫外波段,随着掺杂浓度的增加,吸收限发生“蓝移”。在近红外波段(800-1100nm)1wt.%的ZnO:Al透光率明显高于2wt.%、3wt.%的ZnO:Al薄膜。这主要是因为1wt.% ZnO:Al的载流子浓度低,自由载流子对光子的吸收少引起的。
(3)选取Al掺杂量不同的ZnO:Al薄膜样品(电阻率相同),利用Hall效应测试探究铝掺杂量对薄膜载流子浓度和载流子迁移率的影响。实验得出：在三个样品电阻率大致相同的情况下,随着掺杂量的增加,薄膜的载流子浓度逐渐增加,但薄膜载流子的迁移率逐渐下降。我们从掺杂机制和迁移率的散射机制方面给予解释。
(4)采用2wt.%Al掺杂的陶瓷靶材制备ZnO:Al薄膜,研究氧气流量和衬底温度对薄膜光电性能的影响,同时与2wt.%Al掺杂的合金靶材制备的ZnO:Al薄膜比较衬底温度对它们电阻率的影响。实验得出：①薄膜电阻率随着氧气流量的增加急剧增大。当氧气流量为0.22sccm时,薄膜电阻率最小为5.02×104/Ω·cm,载流子浓度为4.237×1020/cm-3,迁移率29.32cm2/V·s。②薄膜电阻率随着衬底温度的升高逐渐降低。当衬底温度为400℃时,电阻率达到最低4.7×10-4Ω·cm.③与2wt.%Al掺杂的合金靶材制备的ZnO:Al薄膜比较得出：合金靶材制备的ZnO:Al薄膜所需衬底温度较低,当在210℃时,电阻率达到最低最低6.74×10-4Ω·cm.我们从合金靶材反应溅射和陶瓷靶材的溅射机理方面给予解释。
(5)系统研究了1wt.%Al掺杂的ZnO:Al薄膜电阻率受衬底温度的影响,并且将其作为阳极应用到OLED器件中。实验得出：①当衬底温度为230℃时,电阻率最小,阻值为6×10-4Ω·cm。②与相同电阻率的ITO阳极制备的OLED器件对比看出,两种器件都表现出典型的二极管特性。但是从电流密度、发光亮度和电流效率三方面角度来看,AZO薄膜阳极器件均低于ITO薄膜阳极器件的性能。初步分析原因是AZO薄膜的功函数略小于ITO薄膜的功函数,导致阳极空穴注入能力相对降低。
Recently,Al doped ZnO film (ZnO:Al) is a promising transparent conductive film because of its satisfactory electrical and optical properties, low cost of raw materials and stability in hydrogen plasma environment.
ZnO:Al thin film as electrode materials commonly used in photovoltaic devices and OLED devices. Low resistivity and high visible light transmittance are two important factors which can impact on electrode materials. In order to reduce the film resistivity, usually make an appropriate amount of aluminum ions into the ZnO lattice. Aluminum doping content increases concentration of crystal free carrier, thereby enhancing the conductivity properties of ZnO thin films. If the Al doping level is low, the film conductivity can not increase; if Al doping is too high, the excess Al atoms into the lattice not only reduce the carrier concentration and mobility, but also as a lattice scattering Center lower film transmittance in visible region. Can be seen only in the amount of aluminum doping range, can the film both excellent optical and electrical properties. Therefore, the inquiry on Al doped ZnO:Al thin film optical properties is particularly important.
In this paper, the transparent and conductive AZO films were deposited on glass substrate by DC reactive magnetron sputtering from Zn/Al alloy targets doped with 1,2 and 3wt.%and ZnO/Al2O3 ceramic target doped with 2wt.% Al2O3, respectively. The effect of deposition parameters on the structural, electrical and optical properties of AZO films was investigated systematically by scanning electron microscopy (SEM), PANalytical x-ray diffractometry (XRD), four point probe,UV-VIS-IR spectrophotometry and HMS-3000 Hall effect measurement system,respectively. The results indicate:
(1) Effect of substrate temperature on the electrical properties of ZnO:Al thin films with different Al-doped content was investigated. The results showed that with the increasing dopant content the substrate's optimum reaction temperture lowers,at 230℃,210℃,180℃when the resistivity corresponds to a minimum. Respectively, 6.3×10-4Ω·cm、7×10-4Ω·cm and 1×10-3Ω·cm.
(2) Select the same resistivity of ZnO.Al thin film samples with different Al-doped content to study the optical properties. The results showed that in the UV band the blue shifts of the optical absorption edge occurred with the increasing doping concentration. Moreover, in the near-infrared band (800-1100nm) 1wt.% transmittance of AZO was significantly higher than 2,3wt.% of the films. This is mainly because high carrier concentration produces undesirable infrared (IR) absorption by free carriers.
(3) Select the same resistivity of ZnO:Al thin film samples with different Al-doped content to study the electrical properties include carrier concentration and carrier mobility rate by HMS-3000 Hall effect measurement system. The results showed that as the doping increases, the film carrier concentration gradually increased, but the film carrier mobility rate gradually decreased. We mixed scattering mechanism and the mobility of mechanisms to give an explanation.
(4) With 2wt.% Al-doped ceramic target preparation of ZnO:Al thin films to study the substrate temperature on the thin film photovoltaic performance. The results showed that with the substrate temperature increasing, the film resistivity decreased gradually. When the substrate temperature is 390℃, the resistance reached the lowest rate of 4.7×10-4Ω·cm. Then with 2wt.% Al alloy target prepared doped ZnO:Al thin-film comparison of temperature on the resistivity of their impact. The results showed that the ceramic target of the AZO thin films prepared by different alloy target prepared AZO films when the substrate temperature is 210℃, the lowest resistivity of up to 6.74×10-4Ω·cm. Once the deviation from this temperature resistivity of the will increase. We are from the alloy target by reactive sputtering, and ceramic target in the sputtering mechanism to give an explanation.
(5) Systematic study of substrate temperature on lwt.% ZnO:Al thin film resistivityobtained when the substrate temperature of 230℃, the resistivity minimum, resistance to 6×10-4Ω·cm. Then, this sample as an anode applied to the OLED device, and with the same resistivity of the ITO anode prepared by the efficiency of OLED devices for comparison. The results showed that both devices showed typical diode characteristics. However, from the current density, luminance and current efficiency point of view of three aspects, AZO thin film devices are less than the ITO thin film anode anode device performance. The reason is a preliminary analysis of the work function of AZO thin films slightly less than the work function of ITO thin films, leading to the anode hole injection capacity and relatively cheap.
引文
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