硅基稀土掺杂氧化物半导体薄膜电致发光器件
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摘要
众所周知,硅是间接带隙半导体,其极低的发光效率严重限制了硅基光电集成的发展。近二十年来,人们提出了多种途径实现硅基发光。其中,硅基稀土掺杂半导体薄膜的电致发光是一条重要的途径,这是由于稀土发光具有发光谱带窄、波段分布区域宽、光色纯度高且几乎不受外部环境影响等优点。氧化物半导体中稀土离子的固溶度高,且其富氧环境有利于稀土离子的光学跃迁。此外,氧化物半导体薄膜的制备工艺可与集成电路工艺相兼容。因此,若能实现硅基稀土掺杂氧化物半导体薄膜的电致发光,将为硅基发光器件的发展提供新的途径。本文详细研究了硅基稀土掺杂ZnO和TiO2薄膜器件的电致发光及其物理机制,取得的主要创新成果如下：
(1)利用射频溅射法在重掺硼硅(p+-Si)上沉积掺Er的ZnO(ZnO：Er)薄膜,制备出基于ZnO:Er/p+-Si异质结的器件。该器件在不低于6V的直流偏压驱动下,产生源于Er3+离子的-1.54μm电致发光,同时伴有源于ZnO基体的近带边复合紫外发光和缺陷态可见发光。研究表明,掺Er量为0.9at%的器件的-1.54μm电致发光比掺Er量为1.7at%的器件更强,表现出Er浓度淬灭效应。分析指出,与Er3+离子相关的-1.54μm电致发光是由ZnO基体中的缺陷辅助间接复合传递给ZnO晶粒中Er3+离子的能量所激发的。
(2)利用射频溅射法在硅衬底上制备了基于MgxZn1-xO/ZnO:RE异质结的器件。分别采用ZnO:Eu、ZnO:Er和ZnO:Tm薄膜作为发光层,实现了红、绿和蓝三基色电致发光,其启动电压仅为5V左右。此外,分别利用ZnO:Nd和ZnO:Er薄膜作为发光层还实现了中心波长为-0.91gm、-1.09μm和-1.54μm的近红外电致发光。研究发现,器件发光是由注入至MgxZn1-xO势垒层中的空穴被电场加速成为“热空穴”,随后进入ZnO:RE层中直接碰撞激发RE3+离子而产生的。该器件所采用的将热载流子产生层与碰撞激发稀土离子发光层在空间上加以分离的设计思路可应用于开发低电压驱动稀土掺杂半导体薄膜电致发光器件。
(3)利用射频溅射法在p+-Si上沉积掺Er的TiO2(TiO2:Er)薄膜,制备出基于TiO2:Er/p+-Si异质结的发光器件。在不低于5.5V的直流电压驱动下,器件产生源于Er3+离子的可见光区(-522、553、564和663nm)以及红外光区-1.54μm的电致发光。研究发现,在Ti02基体中有足够多的氧空位对激发Er3+离子相关的电致发光至关重要。器件的与Er3+离子相关的电致发光是由Ti02基体中与氧空位相关的束缚激子复合向Er3+离子传递的能量所激发的。
(4)利用射频溅射法在p+-Si上沉积A1和Er共掺的TiO2(TiO2:Al,Er)薄膜,制备出基于TiO2:(Al,Er)/p+-si异质结的电致发光器件。与基于TiO2:Er/p+-Si异质结的器件相比,共掺Al的器件在可见光区的与Er3+离子相关的电致发光被显著抑制,而在红外光区-1.54μm的电致发光得到增强。研究表明,掺Al并未明显改变Ti02基体中的氧空位浓度以及掺入Ti02晶粒中的Er3+离子浓度,即：Al的共掺并未明显改变与Ti02基体向Er3+离子的能量传递相关的供体和受体的数量。因此,如上所述的对Er3+离子电致发光的调控与A1的共掺对Ti02中Er3+离子周围晶体场的影响有关。
(5)利用射频溅射法在p+-Si上沉积掺Nd的TiO2(TiO2:Nd)薄膜,制备出基于TiO2:Nd/p+-Si异质结的发光器件。在不低于5V的直流电压驱动下,器件产生源于Nd3+离子的～0.91、1.09和1.37μm的红外电致发光。研究发现,基于单一锐钛矿相的TiO2:Nd(1.1%)薄膜的异质结器件产生较强的源于TiO2基体的可见发光和相当弱的与Nd3+离子相关的红外发光；而基于锐钛矿和金红石两相共存的TiO2:Nd(2.0%)薄膜的异质结器件的与Nd3+离子相关的红外电致发光得到了显著增强,源于Ti02基体的可见发光被淬灭。实验证实金红石相Ti02中的Nd3+离子不具有光学活性,与锐钛矿Ti02中的Nd3+离子截然相反。分析认为锐钛矿/金红石Ti02两相间的界面态是向锐钛矿Ti02中的Nd3+离子传递能量的有效媒介,它们显著增强了器件的与Nd3+离子相关的红外电致发光。
It is well known that the low luminescence efficiency of silicon (Si) due to its indirect bandgap in nature hinders the development of Si-based optoelectronic integration. In the past two decades, a variety of stratergies have been presented to achieve Si-based light-emitting devices (LEDs). The electroluminescence (EL) from Si-based rare-earth (RE) doped semiconductor devices has received intensive attention. The RE-related luminescences feature narrow linewidths, wide spectral range and weak influence from external environment. Oxide semiconductors have the advantages of high RE solubility and the natural oxygen inclusion which is favorable for optical transition in RE3+ions. Moveover, the preparative processes for oxide semiconductor film are compatible with Si integrated circuit manufacturation. In this context, if the EL from Si-based RE-doped oxide semiconductor thin film devices is achieved, it will offer a new strategy to develop Si-based optoelectronic devices. In this dissertation, the EL performances and related physical mechanisms for Si-based LEDs based on RE-doped ZnO or TiO2films have been intensively investigated. The primary achievements are described as follows.
(1) The LEDs based on the ZnO:Er/p+-Si heterostructures have been prepared, in which the Er-doped ZnO films are deposited by radio frequency (RF) sputtering. At a bias voltage not less than6V, the Er-related～1.54μm EL can be enabled, together with the ultraviolet emission arisen from near-band-edge recombination and visible emissions related to defects in the ZnO host. The～1.54μm EL from the ZnO:Er(0.9%)/p+-Si heterostructured device is stronger than the device using ZnO:Er(1.7%) film, showing the Er-concentration quenching effect. The Er-related～1.54μm EL is triggered by transfer of the energy released from the defect-assisted indirect recombination in the ZnO host to the incorporated Er3+ions.
(2) The LEDs based on the MgxZn1-xO/ZnO:RE heterostructures on Si substrates have been achieved by RF sputtering. Remarkable red, green and blue EL are realized from the devices using the ZnO:Eu, ZnO:Er and ZnO:Tm films as the light-emitting layers, respectively. The threshold voltages are～5V. Moreover, the infrared (IR)(～0.91μm,～1.09μm and～1.54μm) EL can be achieved by using the ZnO:Nd and ZnO:Er films, respectively. The holes injected into the MgxZn1-xO barrier layer are accelerated by the electric field thus becoming the'hot holes', then they enter into the ZnO:RE film to directly impact-excite the RE3+ions, leading to the characteristic emissions. The strategy of spatially separating the hot-carrier generation and impact excitation of RE3+ions is viable to develop low-voltage driven EL devices based on the RE-doped semiconductor films.
(3) The LEDs based on the TiO2:Er/p+-Si heterostructures have been prepared, in which the Er-doped TiO2films are deposited by RF sputtering. The Er-related visible (-522,553,564and663nm) and IR (～1.54μm) EL can be enabled at a bias voltage not less than5.5V. The existence of sufficient oxygen vacancies in TiO2host is critical for the Er-related EL. The energy transfer from the recombination of the trapped-excitons related to oxygen vacancies in TiO2host to Er3+ions triggers the Er-related EL.
(4) The LEDs based on the TiO2:(Al,Er)/p+-Si heterostructures have been prepared, in which the (Al,Er) co-doped TiO2films are deposited by RF sputtering. In comparison with the TiO2:Er/p+-Si heterostructured device, the TiO2:(Al,Er)/p+-Si heterostructured device features the Er-related EL with the substantially suppressed visible emissions and the enhanced～1.54μm IR emission. The Al co-doping is proved not to substantially affect the amounts of the oxygen vacancies in TiO2and the Er3+ions doped into TiO2grains. That is, the quantities of both the sensitizers and activators in the energy transfer from TiO2to Er3+ions are almost consistent. Thus the above-mentioned engineering of Er-related EL is tentatively ascribed to the modification of the crystal field around Er3+ions by the Al co-doping in TiO2.
(5) The LEDs based on the TiO2:Nd/p+-Si heterostructures have been demonstrated, in which the Nd-doped TiO2film are deposited by RF sputtering. The Nd-related IR EL (-0.91,1.09and1.37μm) can be enabled at a bias voltage not less than5V. The device using the TiO2:Nd(1.1%) film of single anatase phase exhibits considerably weak Nd-related EL accompanied with relatively stronger visible emissions from the TiO2host itself. While, the device with the TiO2:Nd(2.0%) film in which the TiO2host coexists with anatase and rutile phases features only pronounced Nd-related EL. It is proved the Nd3+ions in rutile TiO2are not luminescent, quite other than those in anatase TiO2. The anatase/rutile interface states are believed to be the effective mediators in the energy transfer from anatase TiO2to Nd3+ions, leading to the pronounced Nd-related IR EL.
(1)利用射频溅射法在重掺硼硅(p+-Si)上沉积掺Er的ZnO(ZnO：Er)薄膜,制备出基于ZnO:Er/p+-Si异质结的器件。该器件在不低于6V的直流偏压驱动下,产生源于Er3+离子的-1.54μm电致发光,同时伴有源于ZnO基体的近带边复合紫外发光和缺陷态可见发光。研究表明,掺Er量为0.9at%的器件的-1.54μm电致发光比掺Er量为1.7at%的器件更强,表现出Er浓度淬灭效应。分析指出,与Er3+离子相关的-1.54μm电致发光是由ZnO基体中的缺陷辅助间接复合传递给ZnO晶粒中Er3+离子的能量所激发的。
(2)利用射频溅射法在硅衬底上制备了基于MgxZn1-xO/ZnO:RE异质结的器件。分别采用ZnO:Eu、ZnO:Er和ZnO:Tm薄膜作为发光层,实现了红、绿和蓝三基色电致发光,其启动电压仅为5V左右。此外,分别利用ZnO:Nd和ZnO:Er薄膜作为发光层还实现了中心波长为-0.91gm、-1.09μm和-1.54μm的近红外电致发光。研究发现,器件发光是由注入至MgxZn1-xO势垒层中的空穴被电场加速成为“热空穴”,随后进入ZnO:RE层中直接碰撞激发RE3+离子而产生的。该器件所采用的将热载流子产生层与碰撞激发稀土离子发光层在空间上加以分离的设计思路可应用于开发低电压驱动稀土掺杂半导体薄膜电致发光器件。
(3)利用射频溅射法在p+-Si上沉积掺Er的TiO2(TiO2:Er)薄膜,制备出基于TiO2:Er/p+-Si异质结的发光器件。在不低于5.5V的直流电压驱动下,器件产生源于Er3+离子的可见光区(-522、553、564和663nm)以及红外光区-1.54μm的电致发光。研究发现,在Ti02基体中有足够多的氧空位对激发Er3+离子相关的电致发光至关重要。器件的与Er3+离子相关的电致发光是由Ti02基体中与氧空位相关的束缚激子复合向Er3+离子传递的能量所激发的。
(4)利用射频溅射法在p+-Si上沉积A1和Er共掺的TiO2(TiO2:Al,Er)薄膜,制备出基于TiO2:(Al,Er)/p+-si异质结的电致发光器件。与基于TiO2:Er/p+-Si异质结的器件相比,共掺Al的器件在可见光区的与Er3+离子相关的电致发光被显著抑制,而在红外光区-1.54μm的电致发光得到增强。研究表明,掺Al并未明显改变Ti02基体中的氧空位浓度以及掺入Ti02晶粒中的Er3+离子浓度,即：Al的共掺并未明显改变与Ti02基体向Er3+离子的能量传递相关的供体和受体的数量。因此,如上所述的对Er3+离子电致发光的调控与A1的共掺对Ti02中Er3+离子周围晶体场的影响有关。
(5)利用射频溅射法在p+-Si上沉积掺Nd的TiO2(TiO2:Nd)薄膜,制备出基于TiO2:Nd/p+-Si异质结的发光器件。在不低于5V的直流电压驱动下,器件产生源于Nd3+离子的～0.91、1.09和1.37μm的红外电致发光。研究发现,基于单一锐钛矿相的TiO2:Nd(1.1%)薄膜的异质结器件产生较强的源于TiO2基体的可见发光和相当弱的与Nd3+离子相关的红外发光；而基于锐钛矿和金红石两相共存的TiO2:Nd(2.0%)薄膜的异质结器件的与Nd3+离子相关的红外电致发光得到了显著增强,源于Ti02基体的可见发光被淬灭。实验证实金红石相Ti02中的Nd3+离子不具有光学活性,与锐钛矿Ti02中的Nd3+离子截然相反。分析认为锐钛矿/金红石Ti02两相间的界面态是向锐钛矿Ti02中的Nd3+离子传递能量的有效媒介,它们显著增强了器件的与Nd3+离子相关的红外电致发光。
It is well known that the low luminescence efficiency of silicon (Si) due to its indirect bandgap in nature hinders the development of Si-based optoelectronic integration. In the past two decades, a variety of stratergies have been presented to achieve Si-based light-emitting devices (LEDs). The electroluminescence (EL) from Si-based rare-earth (RE) doped semiconductor devices has received intensive attention. The RE-related luminescences feature narrow linewidths, wide spectral range and weak influence from external environment. Oxide semiconductors have the advantages of high RE solubility and the natural oxygen inclusion which is favorable for optical transition in RE3+ions. Moveover, the preparative processes for oxide semiconductor film are compatible with Si integrated circuit manufacturation. In this context, if the EL from Si-based RE-doped oxide semiconductor thin film devices is achieved, it will offer a new strategy to develop Si-based optoelectronic devices. In this dissertation, the EL performances and related physical mechanisms for Si-based LEDs based on RE-doped ZnO or TiO2films have been intensively investigated. The primary achievements are described as follows.
(1) The LEDs based on the ZnO:Er/p+-Si heterostructures have been prepared, in which the Er-doped ZnO films are deposited by radio frequency (RF) sputtering. At a bias voltage not less than6V, the Er-related～1.54μm EL can be enabled, together with the ultraviolet emission arisen from near-band-edge recombination and visible emissions related to defects in the ZnO host. The～1.54μm EL from the ZnO:Er(0.9%)/p+-Si heterostructured device is stronger than the device using ZnO:Er(1.7%) film, showing the Er-concentration quenching effect. The Er-related～1.54μm EL is triggered by transfer of the energy released from the defect-assisted indirect recombination in the ZnO host to the incorporated Er3+ions.
(2) The LEDs based on the MgxZn1-xO/ZnO:RE heterostructures on Si substrates have been achieved by RF sputtering. Remarkable red, green and blue EL are realized from the devices using the ZnO:Eu, ZnO:Er and ZnO:Tm films as the light-emitting layers, respectively. The threshold voltages are～5V. Moreover, the infrared (IR)(～0.91μm,～1.09μm and～1.54μm) EL can be achieved by using the ZnO:Nd and ZnO:Er films, respectively. The holes injected into the MgxZn1-xO barrier layer are accelerated by the electric field thus becoming the'hot holes', then they enter into the ZnO:RE film to directly impact-excite the RE3+ions, leading to the characteristic emissions. The strategy of spatially separating the hot-carrier generation and impact excitation of RE3+ions is viable to develop low-voltage driven EL devices based on the RE-doped semiconductor films.
(3) The LEDs based on the TiO2:Er/p+-Si heterostructures have been prepared, in which the Er-doped TiO2films are deposited by RF sputtering. The Er-related visible (-522,553,564and663nm) and IR (～1.54μm) EL can be enabled at a bias voltage not less than5.5V. The existence of sufficient oxygen vacancies in TiO2host is critical for the Er-related EL. The energy transfer from the recombination of the trapped-excitons related to oxygen vacancies in TiO2host to Er3+ions triggers the Er-related EL.
(4) The LEDs based on the TiO2:(Al,Er)/p+-Si heterostructures have been prepared, in which the (Al,Er) co-doped TiO2films are deposited by RF sputtering. In comparison with the TiO2:Er/p+-Si heterostructured device, the TiO2:(Al,Er)/p+-Si heterostructured device features the Er-related EL with the substantially suppressed visible emissions and the enhanced～1.54μm IR emission. The Al co-doping is proved not to substantially affect the amounts of the oxygen vacancies in TiO2and the Er3+ions doped into TiO2grains. That is, the quantities of both the sensitizers and activators in the energy transfer from TiO2to Er3+ions are almost consistent. Thus the above-mentioned engineering of Er-related EL is tentatively ascribed to the modification of the crystal field around Er3+ions by the Al co-doping in TiO2.
(5) The LEDs based on the TiO2:Nd/p+-Si heterostructures have been demonstrated, in which the Nd-doped TiO2film are deposited by RF sputtering. The Nd-related IR EL (-0.91,1.09and1.37μm) can be enabled at a bias voltage not less than5V. The device using the TiO2:Nd(1.1%) film of single anatase phase exhibits considerably weak Nd-related EL accompanied with relatively stronger visible emissions from the TiO2host itself. While, the device with the TiO2:Nd(2.0%) film in which the TiO2host coexists with anatase and rutile phases features only pronounced Nd-related EL. It is proved the Nd3+ions in rutile TiO2are not luminescent, quite other than those in anatase TiO2. The anatase/rutile interface states are believed to be the effective mediators in the energy transfer from anatase TiO2to Nd3+ions, leading to the pronounced Nd-related IR EL.
引文
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