酞菁铜单晶微纳场效应晶体管在气体传感器中的应用基础研究
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摘要
有机半导体场效应晶体管气体传感器相比于电阻式器件，由于具有灵敏度高、室温工作、易于集成以及独立的多参数等优点在气体传感器领域一直倍受人们关注。目前国际上报道的薄膜或微纳单晶场效应晶体管气体传感器都采用固体绝缘层。因此，半导体/绝缘层接触界面上不可避免的发生载流子束缚、电荷掺杂、分子（或原子）重构、偶极子的形成以及一些可能的化学相互作用，从而降低传感器的性能及稳定性。更主要的是固体绝缘层遮蔽了大部分对吸附分子最为敏感的导电沟道界面，影响了场效应晶体管气体传感器灵敏度的进一步提高。因此，如果把固态绝缘层用空气间隙来替代构筑器件，开展研究，不仅能保证半导体和绝缘层的良好的接触界面，提高器件性能、稳定性以及成功率，同时提供被测气体分子直接影响场效应晶体管最为敏感的导电沟道的通道。有望在灵敏度、响应速度和检测极限上获得突破。并且，采用微纳单晶材料有利于工作机理的探讨，为推动场效应晶体管型气体传感器的进一步发展和应用提供理论指导。
酞菁铜不仅具有良好的化学、热稳定性，同时具有卓越的气敏特性，在有机气体传感器研究中倍受关注。本论文以酞菁铜为代表开展了酞菁铜单晶微纳场效应晶体管在气体传感器中的应用基础研究。主要内容如下：
1.进行了酞菁铜单晶微纳场效应晶体管气体传感器在SO_2检测中的应用基础研究。成功构筑了具有高灵敏度、低检测极限、快速响应及在室温工作条件下完全恢复等优点的空气间隙为绝缘层的酞菁铜单晶微纳场效应晶体管SO_2传感器。其检测极限为0.5ppm，灵敏度和分辨率分别为119%和100ppb。对0.5ppm SO_2的响应-恢复时间分别为3min和8min。据我们所知，这是首次采用有机场效应晶体管作为SO_2气体传感器的报道，并且器件有些传感性能可与商用的化学传感器媲美；通过理论计算与实验结果相结合，研究了此类器件的响应机理。
2．研究了空气间隙绝缘层酞菁铜单晶微纳场效应晶体管的多参数在气体甄别中的应用及其响应机理。提出了利用多参数和真值表结合，利用单个器件甄别NO_2、NO以及SO_2三种有毒有害气体的简单明了的方法。根本原理上提高了半导体气体传感器的选择性。
3.发展了一种提高基于有机单晶场效应晶体管性能的简单、有效的“气体增强法”。通过方法调控场效应晶体管的迁移率，开关闭以及阈值电压等参数。通过实验证实该方法具有一定的普适性。
Organic field effect transistor gas sensors have attracted much attention, because ofseveral advantages over resistors, such as high sensitivity，easy to integrated and reversiblemulti-parametric, apart from the great advantage of being operated at room temperature.However, carrier trapping，charger doping， molecular reorientation，dipole formation，anda range of possible chemical interations are among the many phenomena that can occur at theorganic material/solid dielectric interface and degrade device performance and stability.Moreover, the the most sensitive conductive channel of the traditional solid dielectric FETs iscapped by the semiconductor layer and the solid dielectric, so that the performanceimprovement of the transistors gas sensors are blocked. In contrast, the gas dielectric makesthe conductive channel exposed to the detected gas, which will not only facilitates the directinteraction between the gas molecules and the conductive channel resulting in theimprovement of the sensing performance，but also provides a pristine interface to reduce theinterface defects, weaken the carrier trapping, make the intrinsic charge transport possible,and minimize the Fr hlich polaron effect at the interface and improve device stability. As aresult, we can anticipate that the sensing performance of the sensors should be improved，suchas sensitivity, response and limit of detection etc. Furthermore, sub-micro/nanometer-sizedorganic single crystals can not only futher improvement of sesnsor performance, but alsobeneficial for investigating response mechanism.
CuPc have attracted attention in organic gas sensors not only because of its exceptionalthermal and chemical stability, but also its remarkable gas sensing properties. In thisdissertation, we fabricated an OFET based on gas dielectric and sub-micro/nanometer-sizedCuPc single crystals as novel gas sensors and investigated their gas sensing properties.Themain results are as follows:
1. The room-temperature gas dielectric sub-micro/nanometer-sized CuPc single crystallinefield effect transistor SO_2sensors with high sensitivity, low detection limit, fast response andcomplete recovery have been fabricated. The detect limitation is down to sub ppm levels (0.5ppm) with the sensitivity of119%and high resolution of100ppb. The response and recoverytime are only3and8min in0.5ppm SO_2, respectively. To the best of our knowledge, this isthe first demonstration of SO_2gas sensing based on Organic field effect transistor. Some ofthe sensing performances of this device are comparable to the commercialized solid electrolyte sensors. The theory analysis and comparative experiments between solid and gasdielectric devices show that the exposed conductive channel by gas dielectric is responsiblefor the sensitivity to SO_2.
2. Gas dielectric sub-micro/nanometer-sized CuPc single crystalline field effect transistoras multi-parameter sensors and their response mechanism are investigated. A combination ofmulti-parameter and ture table provides a simple toure to detect NO_2, NO and SO_2selectively.These three gases were distinguished by this method successfully.
3. Developed a new, simple, efficient route to enhancing performance of single crystallineOrganic field effect transistor by “gas enhancing methods”. This method is universallyapplicable.
酞菁铜不仅具有良好的化学、热稳定性，同时具有卓越的气敏特性，在有机气体传感器研究中倍受关注。本论文以酞菁铜为代表开展了酞菁铜单晶微纳场效应晶体管在气体传感器中的应用基础研究。主要内容如下：
1.进行了酞菁铜单晶微纳场效应晶体管气体传感器在SO_2检测中的应用基础研究。成功构筑了具有高灵敏度、低检测极限、快速响应及在室温工作条件下完全恢复等优点的空气间隙为绝缘层的酞菁铜单晶微纳场效应晶体管SO_2传感器。其检测极限为0.5ppm，灵敏度和分辨率分别为119%和100ppb。对0.5ppm SO_2的响应-恢复时间分别为3min和8min。据我们所知，这是首次采用有机场效应晶体管作为SO_2气体传感器的报道，并且器件有些传感性能可与商用的化学传感器媲美；通过理论计算与实验结果相结合，研究了此类器件的响应机理。
2．研究了空气间隙绝缘层酞菁铜单晶微纳场效应晶体管的多参数在气体甄别中的应用及其响应机理。提出了利用多参数和真值表结合，利用单个器件甄别NO_2、NO以及SO_2三种有毒有害气体的简单明了的方法。根本原理上提高了半导体气体传感器的选择性。
3.发展了一种提高基于有机单晶场效应晶体管性能的简单、有效的“气体增强法”。通过方法调控场效应晶体管的迁移率，开关闭以及阈值电压等参数。通过实验证实该方法具有一定的普适性。
Organic field effect transistor gas sensors have attracted much attention, because ofseveral advantages over resistors, such as high sensitivity，easy to integrated and reversiblemulti-parametric, apart from the great advantage of being operated at room temperature.However, carrier trapping，charger doping， molecular reorientation，dipole formation，anda range of possible chemical interations are among the many phenomena that can occur at theorganic material/solid dielectric interface and degrade device performance and stability.Moreover, the the most sensitive conductive channel of the traditional solid dielectric FETs iscapped by the semiconductor layer and the solid dielectric, so that the performanceimprovement of the transistors gas sensors are blocked. In contrast, the gas dielectric makesthe conductive channel exposed to the detected gas, which will not only facilitates the directinteraction between the gas molecules and the conductive channel resulting in theimprovement of the sensing performance，but also provides a pristine interface to reduce theinterface defects, weaken the carrier trapping, make the intrinsic charge transport possible,and minimize the Fr hlich polaron effect at the interface and improve device stability. As aresult, we can anticipate that the sensing performance of the sensors should be improved，suchas sensitivity, response and limit of detection etc. Furthermore, sub-micro/nanometer-sizedorganic single crystals can not only futher improvement of sesnsor performance, but alsobeneficial for investigating response mechanism.
CuPc have attracted attention in organic gas sensors not only because of its exceptionalthermal and chemical stability, but also its remarkable gas sensing properties. In thisdissertation, we fabricated an OFET based on gas dielectric and sub-micro/nanometer-sizedCuPc single crystals as novel gas sensors and investigated their gas sensing properties.Themain results are as follows:
1. The room-temperature gas dielectric sub-micro/nanometer-sized CuPc single crystallinefield effect transistor SO_2sensors with high sensitivity, low detection limit, fast response andcomplete recovery have been fabricated. The detect limitation is down to sub ppm levels (0.5ppm) with the sensitivity of119%and high resolution of100ppb. The response and recoverytime are only3and8min in0.5ppm SO_2, respectively. To the best of our knowledge, this isthe first demonstration of SO_2gas sensing based on Organic field effect transistor. Some ofthe sensing performances of this device are comparable to the commercialized solid electrolyte sensors. The theory analysis and comparative experiments between solid and gasdielectric devices show that the exposed conductive channel by gas dielectric is responsiblefor the sensitivity to SO_2.
2. Gas dielectric sub-micro/nanometer-sized CuPc single crystalline field effect transistoras multi-parameter sensors and their response mechanism are investigated. A combination ofmulti-parameter and ture table provides a simple toure to detect NO_2, NO and SO_2selectively.These three gases were distinguished by this method successfully.
3. Developed a new, simple, efficient route to enhancing performance of single crystallineOrganic field effect transistor by “gas enhancing methods”. This method is universallyapplicable.
引文
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