无机双电层栅介质及其低电压氧化物微纳晶体管应用
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摘要
基于氧化物半导体的微纳晶体管,由于其制备温度低、高电子迁移率等独特优势在平板显示、电子纸、传感器等领域具有广泛的应用价值。常规器件采用的热氧化SiO2栅介质由于其低介电常数导致较弱的栅电极/沟道耦合作用,工作电压一般都大于20V。较高的工作电压对于低功耗的便携式电子产品应用是个巨大的障碍。本研究论文主要研究基于具有双电层效应的SiO2固态电解质的全无机低电压氧化物微纳晶体管,包括薄膜晶体管和纳米线晶体管。并在以下几个方面取得了突出的研究成果：
(1)通过特殊的等离子体化学汽相沉积(PECVD)工艺制备了具有高双电层单位电容的SiO2固态电解质,并且对SiO2固态电解质的极化机理进行了详细的研究。在不同频率下SiO2具有三种不同的极化：双电层形成(低频),离子迁移(中频)以及偶极子极化(高频)。通过改变SiO2固态电解质的制备条件,我们改善了SiO2固态电解质的极化响应速度,120℃C沉积的SiO2固态电解质在1kHz时双电层电容高达1μF/cm2,在10kHz时仍高达0.6μF/cm2。分析了不同温度下Si02固态电解质的形貌。同时我们利用SiO2固态电解质制备了In-Zn-O薄膜晶体管,其工作电压降低到1V以内。器件的场效应电子迁移率,电流开关比以及亚阈值斜率分别为46.2cm2/Vs,106和69mV/decade。由于SiO2固态电解质具有快速的极化响应时间,因此基于该栅介质的In-Zn-O薄膜晶体管有望具有kHz的开关频率。
(2)制备了SiO2质子导体以及利用单掩模自组装法制备了基于SiO2质子导体的In-Zn-O共面同质结透明薄膜晶体管,并对其电学特性和光学特性进行了研究。随着磷酸溶液浓度从0%增加到50%,SiO2质子导体在20Hz的单位电容逐渐增加,最大为8μF/cm2。并且器件的双电层形成的上限频率逐渐升高。随着磷酸溶液浓度的增加,器件的饱和迁移率、工作电压、亚阈值摆幅、阈值电压和开关电流比都会发生不同程度的变化。变化最明显的是器件的工作电压,随着磷酸溶液浓度的增加,器件的工作电压从1.5V降低到0.6V,器件的亚阈值斜率也逐渐的减小到68mV/decade。器件的迁移率为12cm2/Vs。器件的光学透光特性优异,其透光率高达75%以上。
(3)研制了基于SiO2固态电解质的纸张薄膜晶体管(Sb掺杂SnO2和InGaZnO4沟道)及其通过氧压调制技术实现不同工作模式的薄膜晶体管。首先,我们制备了基于SiO2固态电解质的电池可驱动的低电压Sb掺杂SnO2纸张薄膜晶体管,由于SiO2固态电解质具有形成双电层的能力,因而器件的栅介质单位电容在40Hz时高达1.36μF/cm2,纸张器件的工作降低到1.5V以内,并且器件的阈值电压接近于0V(Vth=0.06V)。纸张器件的具有优异的电学特性,其亚阈值斜率,电流开关比和饱和场效应电子迁移率分别为-80mV/decade,大于105和21cm2/Vs。这是世界上报道过的最低工作电压的纸张薄膜晶体管。同时,我们还在纸张衬底上制备了低电压In-Ga-Zn-O薄膜晶体管,通过阻抗谱以及傅里叶转换红外光谱表征了SiO2的固态电解质特性。最重要的是,我们通过氧压调制技术改变了In-Ga-Zn-O的沟道电导,从而实现了耗尽模式(Vth=-0.45)和增强模式(Vth=0.25V)的低电压In-Ga-Zn-O纸张薄膜晶体管。
(4)引入了全新的单根纳米线晶体管的制作工艺,不需要采用任何的光刻技术。我们发展了一种镍网掩模技术制备全透明的单根Sb掺杂8nO2纳米线晶体管在没有热退火和表面钝化的情况下,纳米线的表面损伤可以避免,这种方法非常有利于一维无机纳米线材料的光电特性研究。制备的Sb掺杂SnO2纳米线晶体管是利用高单位电容的SiO2固态电解质作为栅介质(2μF/cm2),其工作电压降低到1.5V。器件的饱和电子迁移率、电流开关比以及亚阈值斜率分别为175cm2/Vs,105和116mV/decade。动态和静态偏压应力测试证明我们的单根Sb掺杂SnO2纳米线透明晶体管能够持续的运行在低电压并保持极好的稳定性和重复性。
(5)研究了基于SiO2固态电解质的In-Zn-O薄膜晶体管的不规则阈值电压漂移以及表面钝化对其电学性能的影响。没有经过表面钝化的器件在短时间的光照和负偏压应力条件下出现较大负阈值电压漂移(0.68V)。经过长时间的负偏压应力测试,没有钝化和已经钝化的器件都出现不规则的正阈值电压漂移,这主要是由于SiO2固态电解质中离子漂移现象产生的。经过表面钝化以后,器件的负阂值电压小于0.1V,这主要是由于经过表面钝化以后器件的光解吸附氧离子的现象得到抑制。
(6)利用自主设计的掩模板,通过单掩模自组装法制备了具有新型双栅结构的低电压纸张薄膜晶体管。该双栅纸张薄膜晶体管具有底栅和共平面栅两个栅极。并且我们对共平面栅极对双栅纸张薄膜晶体管的电学特性影响进行了研究。当共平面栅极电压从2V变化到-2V时,纸张薄膜晶体管的阈值电压从-0.98V变化到0.94V。制备的纸张薄膜晶体管具有高性能,在不同的共平面栅极电压下,电流开关比为6×105,亚阈值斜率为0.14-0.19V/decade,以及饱和场效应电子迁移率为8.64-9.45cm2/Vs。
Oxide semiconductor-based micro/nanotransistors have potential applications in flat-panel displays, E-paper and chemical-biological sensors because of their low processing temperature and high electron mobility. Traditional transistors are gated by themally grown SiO2which shows high operating voltage because of the week gate coupling of such dielectrics. It is not compitable with the portable electronics. In this dissertation, inorganic low-voltage oxide-based micro/nanotransistors gated by SiO2solid electrolyte with electric-double-layer (EDL) effect were stuied, including thin-film transistors (TFTs) and nanowire transistors. The obtained results are summarized below.
(1) SiO2solid electrolytes with high specific EDL capacitance were deposited by specific plasma enhanced chemical vapor deposition (PECVD) technology. The polarization mechnisim of a SiO2solid electroclyte was developed. Three polarizations are indentified at different:EDL formation (low frequencies), ionic relaxation (intermediate frequencies) and dipole relaxation (high frequencies). The polarization response of the SiO2solid electroclyte was optimized by changing the deposition condition and the improved specific capacitance is1μF/cm2at1kHz and remains0.6μF/cm2at10kHz. We have also stuied the morphology of SiO2solid electrolyte. Ultralow-voltage (<1V) transparent In-Zn-O TFTs gated by such dielectrics were fabricated. The field-effect mobility, current on/off ratio and subthreshold swing were estimated to be46.2cm2/Vs,106and69mV/decade. Such TFTs hold promise to perate at1kHz because of the fast polarization response of the SiO2solid electroclyte.
(2) The SiO2-based proton conductors and transparent In-Zn-O coplanar homojunction TFTs gated by such dielectrics were prepared. As the H3PO4concentration changed from0%to50%, the specific EDL capacitance of the SiO2-based proton conductors and the upper frequency limit of EDL formation were increased, and the field-effect mobility, operating voltage, subthreshold swing and current on/off ratio were also changed. The operating voltage of such TFTs was changed from1.5V to0.6V as the H3PO4concentration increased. The transparent high performance In-Zn-O TFTs with a field-effect mobility of12cm2/Vs and a average transmittance of75%were obtained.
(3) The paper TFTs (Sb-doped SnO2and InGaZnO4channels) gated by SiO2solid electrolyte were fabricated and the operation mode of such devices were tuing by oxygen-modulation technology. Battery drivable low-voltage sb-doped SnO2-based paper TFTs with a near-zero threshold voltage (Vth=0.06V) gated by microporous SiO2dielectric with EDL effect were firstly fabricated by our group. The operating voltage is found to be as low as1.5V due to the huge gate specific capacitance (1.34μF/cm2at40Hz) related to EDL formation. The subthreshold gate voltage swing, current on/off ratio and field-effect mobility were found to be<80mV/decade,>105and>21cm2/Vs, respectively. InGaZnO4thin-film transistors (TFTs) on paper substrates gated by SiO2solid electrolyte were fabricated at room temperature and the impedance spectroscopy (ionic-conductivity-frequency and capacitance-voltage characteristics) and Fourier-transformed infrared spectroscopy of SiO2were characterized. Most importantly, both depletion-mode (Vth=-0.45V) and enhancement-mode (Vth=0.25V) operations were realized by rationally controlling the oxygen concentration in argon ambient during InGaZnO4channel deposition.
(4) We introduce a simple nickel grid mask method to fabricate transparent single Sb-doped SnO2nanowire transistors without use of lithographic tools. Damage of the nanowire's surface can be avoided without any thermal annealing and surface modification, which is very convenient for the fundamental electrical and photoelectric characterization of one-dimensional inorganic nanomaterials. The high specific capapcitance (2μF/cm2) SiO2solid electrolyte was used as the gate dielectric which results in the operating voltage was reduced to less than1.5V. The field-effect mobility, current on/off ratio and subthreshold swing were estimated to be175cm2/Vs,105, and116mV/decade, respectively. The static and dynamic bias stress measurements indicate that transparent SnO2nanowire FETs can operate at low-voltage with highly reproducibility.
(5) Threshold voltage (Vth) instability and surface passivation effect of transparent In-Zn-O EDL TFTs were investigated. Unpassivated devices show a large negative threshold voltage shift of0.68V in the beginning of light-illuminated negative gate bias stress. Under longer time stress, anomalous positive Vth shifts were observed for both unpassivated and passivated TFTs, which was due to the mobile ions drifting in the SiO2-based solid-electrolyte gate dielectric. After surface passivation, the devices show neglectable negative Vth shifts of less than0.1V due to the protection of channel against the photodesorption of adsorbed oxygen ions.
(6) Novel double-gate low-voltage paper TFTs were fabricated by self-assembled method. Such paper TFTs have a bottom-gate gate and an in-plane electrode gate and the electrical modulation effect of the in-plane electrode was investigated. The threshold voltage (Vth) of such paper TFTs was tuned from-0.98to0.94V as the voltage biases of the in-plane electrode was changed from2V to-2V. High electrical performance with a current on/off ratio of6×105～106, a subthreshold swing of0.14～0.19V/decade, and a mobility of8.64～9.45cm2/V s was obtained at different in-plane electrode voltage biases.
(1)通过特殊的等离子体化学汽相沉积(PECVD)工艺制备了具有高双电层单位电容的SiO2固态电解质,并且对SiO2固态电解质的极化机理进行了详细的研究。在不同频率下SiO2具有三种不同的极化：双电层形成(低频),离子迁移(中频)以及偶极子极化(高频)。通过改变SiO2固态电解质的制备条件,我们改善了SiO2固态电解质的极化响应速度,120℃C沉积的SiO2固态电解质在1kHz时双电层电容高达1μF/cm2,在10kHz时仍高达0.6μF/cm2。分析了不同温度下Si02固态电解质的形貌。同时我们利用SiO2固态电解质制备了In-Zn-O薄膜晶体管,其工作电压降低到1V以内。器件的场效应电子迁移率,电流开关比以及亚阈值斜率分别为46.2cm2/Vs,106和69mV/decade。由于SiO2固态电解质具有快速的极化响应时间,因此基于该栅介质的In-Zn-O薄膜晶体管有望具有kHz的开关频率。
(2)制备了SiO2质子导体以及利用单掩模自组装法制备了基于SiO2质子导体的In-Zn-O共面同质结透明薄膜晶体管,并对其电学特性和光学特性进行了研究。随着磷酸溶液浓度从0%增加到50%,SiO2质子导体在20Hz的单位电容逐渐增加,最大为8μF/cm2。并且器件的双电层形成的上限频率逐渐升高。随着磷酸溶液浓度的增加,器件的饱和迁移率、工作电压、亚阈值摆幅、阈值电压和开关电流比都会发生不同程度的变化。变化最明显的是器件的工作电压,随着磷酸溶液浓度的增加,器件的工作电压从1.5V降低到0.6V,器件的亚阈值斜率也逐渐的减小到68mV/decade。器件的迁移率为12cm2/Vs。器件的光学透光特性优异,其透光率高达75%以上。
(3)研制了基于SiO2固态电解质的纸张薄膜晶体管(Sb掺杂SnO2和InGaZnO4沟道)及其通过氧压调制技术实现不同工作模式的薄膜晶体管。首先,我们制备了基于SiO2固态电解质的电池可驱动的低电压Sb掺杂SnO2纸张薄膜晶体管,由于SiO2固态电解质具有形成双电层的能力,因而器件的栅介质单位电容在40Hz时高达1.36μF/cm2,纸张器件的工作降低到1.5V以内,并且器件的阈值电压接近于0V(Vth=0.06V)。纸张器件的具有优异的电学特性,其亚阈值斜率,电流开关比和饱和场效应电子迁移率分别为-80mV/decade,大于105和21cm2/Vs。这是世界上报道过的最低工作电压的纸张薄膜晶体管。同时,我们还在纸张衬底上制备了低电压In-Ga-Zn-O薄膜晶体管,通过阻抗谱以及傅里叶转换红外光谱表征了SiO2的固态电解质特性。最重要的是,我们通过氧压调制技术改变了In-Ga-Zn-O的沟道电导,从而实现了耗尽模式(Vth=-0.45)和增强模式(Vth=0.25V)的低电压In-Ga-Zn-O纸张薄膜晶体管。
(4)引入了全新的单根纳米线晶体管的制作工艺,不需要采用任何的光刻技术。我们发展了一种镍网掩模技术制备全透明的单根Sb掺杂8nO2纳米线晶体管在没有热退火和表面钝化的情况下,纳米线的表面损伤可以避免,这种方法非常有利于一维无机纳米线材料的光电特性研究。制备的Sb掺杂SnO2纳米线晶体管是利用高单位电容的SiO2固态电解质作为栅介质(2μF/cm2),其工作电压降低到1.5V。器件的饱和电子迁移率、电流开关比以及亚阈值斜率分别为175cm2/Vs,105和116mV/decade。动态和静态偏压应力测试证明我们的单根Sb掺杂SnO2纳米线透明晶体管能够持续的运行在低电压并保持极好的稳定性和重复性。
(5)研究了基于SiO2固态电解质的In-Zn-O薄膜晶体管的不规则阈值电压漂移以及表面钝化对其电学性能的影响。没有经过表面钝化的器件在短时间的光照和负偏压应力条件下出现较大负阈值电压漂移(0.68V)。经过长时间的负偏压应力测试,没有钝化和已经钝化的器件都出现不规则的正阈值电压漂移,这主要是由于SiO2固态电解质中离子漂移现象产生的。经过表面钝化以后,器件的负阂值电压小于0.1V,这主要是由于经过表面钝化以后器件的光解吸附氧离子的现象得到抑制。
(6)利用自主设计的掩模板,通过单掩模自组装法制备了具有新型双栅结构的低电压纸张薄膜晶体管。该双栅纸张薄膜晶体管具有底栅和共平面栅两个栅极。并且我们对共平面栅极对双栅纸张薄膜晶体管的电学特性影响进行了研究。当共平面栅极电压从2V变化到-2V时,纸张薄膜晶体管的阈值电压从-0.98V变化到0.94V。制备的纸张薄膜晶体管具有高性能,在不同的共平面栅极电压下,电流开关比为6×105,亚阈值斜率为0.14-0.19V/decade,以及饱和场效应电子迁移率为8.64-9.45cm2/Vs。
Oxide semiconductor-based micro/nanotransistors have potential applications in flat-panel displays, E-paper and chemical-biological sensors because of their low processing temperature and high electron mobility. Traditional transistors are gated by themally grown SiO2which shows high operating voltage because of the week gate coupling of such dielectrics. It is not compitable with the portable electronics. In this dissertation, inorganic low-voltage oxide-based micro/nanotransistors gated by SiO2solid electrolyte with electric-double-layer (EDL) effect were stuied, including thin-film transistors (TFTs) and nanowire transistors. The obtained results are summarized below.
(1) SiO2solid electrolytes with high specific EDL capacitance were deposited by specific plasma enhanced chemical vapor deposition (PECVD) technology. The polarization mechnisim of a SiO2solid electroclyte was developed. Three polarizations are indentified at different:EDL formation (low frequencies), ionic relaxation (intermediate frequencies) and dipole relaxation (high frequencies). The polarization response of the SiO2solid electroclyte was optimized by changing the deposition condition and the improved specific capacitance is1μF/cm2at1kHz and remains0.6μF/cm2at10kHz. We have also stuied the morphology of SiO2solid electrolyte. Ultralow-voltage (<1V) transparent In-Zn-O TFTs gated by such dielectrics were fabricated. The field-effect mobility, current on/off ratio and subthreshold swing were estimated to be46.2cm2/Vs,106and69mV/decade. Such TFTs hold promise to perate at1kHz because of the fast polarization response of the SiO2solid electroclyte.
(2) The SiO2-based proton conductors and transparent In-Zn-O coplanar homojunction TFTs gated by such dielectrics were prepared. As the H3PO4concentration changed from0%to50%, the specific EDL capacitance of the SiO2-based proton conductors and the upper frequency limit of EDL formation were increased, and the field-effect mobility, operating voltage, subthreshold swing and current on/off ratio were also changed. The operating voltage of such TFTs was changed from1.5V to0.6V as the H3PO4concentration increased. The transparent high performance In-Zn-O TFTs with a field-effect mobility of12cm2/Vs and a average transmittance of75%were obtained.
(3) The paper TFTs (Sb-doped SnO2and InGaZnO4channels) gated by SiO2solid electrolyte were fabricated and the operation mode of such devices were tuing by oxygen-modulation technology. Battery drivable low-voltage sb-doped SnO2-based paper TFTs with a near-zero threshold voltage (Vth=0.06V) gated by microporous SiO2dielectric with EDL effect were firstly fabricated by our group. The operating voltage is found to be as low as1.5V due to the huge gate specific capacitance (1.34μF/cm2at40Hz) related to EDL formation. The subthreshold gate voltage swing, current on/off ratio and field-effect mobility were found to be<80mV/decade,>105and>21cm2/Vs, respectively. InGaZnO4thin-film transistors (TFTs) on paper substrates gated by SiO2solid electrolyte were fabricated at room temperature and the impedance spectroscopy (ionic-conductivity-frequency and capacitance-voltage characteristics) and Fourier-transformed infrared spectroscopy of SiO2were characterized. Most importantly, both depletion-mode (Vth=-0.45V) and enhancement-mode (Vth=0.25V) operations were realized by rationally controlling the oxygen concentration in argon ambient during InGaZnO4channel deposition.
(4) We introduce a simple nickel grid mask method to fabricate transparent single Sb-doped SnO2nanowire transistors without use of lithographic tools. Damage of the nanowire's surface can be avoided without any thermal annealing and surface modification, which is very convenient for the fundamental electrical and photoelectric characterization of one-dimensional inorganic nanomaterials. The high specific capapcitance (2μF/cm2) SiO2solid electrolyte was used as the gate dielectric which results in the operating voltage was reduced to less than1.5V. The field-effect mobility, current on/off ratio and subthreshold swing were estimated to be175cm2/Vs,105, and116mV/decade, respectively. The static and dynamic bias stress measurements indicate that transparent SnO2nanowire FETs can operate at low-voltage with highly reproducibility.
(5) Threshold voltage (Vth) instability and surface passivation effect of transparent In-Zn-O EDL TFTs were investigated. Unpassivated devices show a large negative threshold voltage shift of0.68V in the beginning of light-illuminated negative gate bias stress. Under longer time stress, anomalous positive Vth shifts were observed for both unpassivated and passivated TFTs, which was due to the mobile ions drifting in the SiO2-based solid-electrolyte gate dielectric. After surface passivation, the devices show neglectable negative Vth shifts of less than0.1V due to the protection of channel against the photodesorption of adsorbed oxygen ions.
(6) Novel double-gate low-voltage paper TFTs were fabricated by self-assembled method. Such paper TFTs have a bottom-gate gate and an in-plane electrode gate and the electrical modulation effect of the in-plane electrode was investigated. The threshold voltage (Vth) of such paper TFTs was tuned from-0.98to0.94V as the voltage biases of the in-plane electrode was changed from2V to-2V. High electrical performance with a current on/off ratio of6×105～106, a subthreshold swing of0.14～0.19V/decade, and a mobility of8.64～9.45cm2/V s was obtained at different in-plane electrode voltage biases.
引文
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