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氧化物雙電層晶體管及其人造突觸和生化傳感應(yīng)用

發(fā)布時(shí)間:2018-05-13 00:17

  本文選題:電解質(zhì) + 雙電層 ; 參考:《中國科學(xué)院寧波材料技術(shù)與工程研究所》2016年博士論文


【摘要】:近年來,由于電解質(zhì)材料具有巨大的雙電層電容效應(yīng),研究人員將電解質(zhì)用作晶體管的柵介質(zhì)材料實(shí)現(xiàn)了低壓工作的晶體管器件。然而此類晶體管器件大部分是基于液體電解質(zhì)柵介質(zhì)和有機(jī)半導(dǎo)體溝道,因此在器件集成和穩(wěn)定性方面存在一定的缺陷。將固態(tài)電解質(zhì)用作氧化物薄膜晶體管的柵介質(zhì)材料,降低器件工作電壓的同時(shí)具有良好的結(jié)構(gòu)擴(kuò)展性和器件穩(wěn)定性,還有助于設(shè)計(jì)新穎的器件結(jié)構(gòu)。此外,電解質(zhì)中獨(dú)特的離子極化響應(yīng)行為和器件界面處極強(qiáng)的離子/電子耦合現(xiàn)象,符合神經(jīng)仿生和生化傳感領(lǐng)域的需求。本論文研究了以海藻酸鈉質(zhì)子導(dǎo)體膜、自支撐殼聚糖質(zhì)子導(dǎo)體膜和SiO_2質(zhì)子導(dǎo)體膜等固態(tài)電解質(zhì)為柵介質(zhì)的氧化物雙電層晶體管,并研究雙電層晶體管在人造突觸和生化傳感等領(lǐng)域的應(yīng)用。本論文的主要工作可以概括為以下幾個(gè)方面:(1)通過簡(jiǎn)單的涂布法制備了海藻酸鈉薄膜,發(fā)現(xiàn)薄膜具有較大的雙電層電容(~4.6μF/cm~2)和高的質(zhì)子電導(dǎo)率(~7.7×10-4 S/cm)。在一定范圍內(nèi)溫度越高相對(duì)濕度越大,海藻酸鈉質(zhì)子導(dǎo)體膜的雙電層電容越大。由于海藻酸鈉質(zhì)子導(dǎo)體膜具有三維質(zhì)子傳導(dǎo)特性,質(zhì)子可在側(cè)向電場(chǎng)下遠(yuǎn)距離遷移,形成側(cè)向的質(zhì)子/電子耦合。我們首次采用海藻酸鈉質(zhì)子導(dǎo)體膜作為柵介質(zhì)成功研制了低壓側(cè)向耦合氧化物雙電層晶體管,器件的電流開關(guān)比~3.1×106、工作電壓1.5 V、閾值電壓為-0.1 V、飽和區(qū)場(chǎng)效應(yīng)遷移率為9.5 cm~2/V·s、亞閾值擺幅為100 m V/dec。并研制了基于海藻酸鈉調(diào)控側(cè)向耦合氧化物雙電層晶體管的電阻負(fù)載型反相器,當(dāng)反相器的電源電壓為1.0 V時(shí),電壓增益高達(dá)5。基于海藻酸鈉調(diào)控側(cè)向耦合氧化物雙電層晶體管的雙側(cè)柵工作模式,實(shí)現(xiàn)與門邏輯功能。最后,在柔性紙張襯底上制備海藻酸鈉質(zhì)子導(dǎo)體紙張氧化物雙電層晶體管,該器件在較低的工作電壓下表現(xiàn)出良好的晶體管性能,并基于雙側(cè)柵模式實(shí)現(xiàn)了與門邏輯功能。(2)采用簡(jiǎn)單的涂布-剝離工藝制備了自支撐殼聚糖薄膜,發(fā)現(xiàn)薄膜具有較大的側(cè)向雙電層電容(~0.7μF/cm~2),實(shí)驗(yàn)結(jié)果表明自支撐殼聚糖薄膜是電子絕緣但質(zhì)子傳導(dǎo)的固態(tài)電解質(zhì)薄膜。我們首次采用自支撐殼聚糖質(zhì)子導(dǎo)體膜作為晶體管的柵介質(zhì)層,成功研制了自支撐柔性氧化物雙電層晶體管。器件的電流開關(guān)比106、工作電壓1.6 V、閾值電壓為-0.2 V、遷移率為14.2 cm~2/V·s、亞閾值擺幅為120 m V/dec,同時(shí)具有良好的穩(wěn)定性和抗彎曲性能。雙電層晶體管作為一種離子/電子雜化晶體管,其電學(xué)特性受到離子遷移和離子/電子界面耦合的影響。生物體內(nèi)的液體環(huán)境充滿著各種離子,神經(jīng)系統(tǒng)內(nèi)的信息傳遞過程同樣存在類似的耦合現(xiàn)象。因此,我們將自支撐柔性氧化物雙電層晶體管作為人造突觸,詳細(xì)研究了該突觸器件的記憶/學(xué)習(xí)、短程/長(zhǎng)程塑性、高通濾波和多輸入時(shí)空信息整合等特性。正向柵壓脈沖刺激下,溝道電流呈現(xiàn)類似生物突觸的EPSC特性;雙脈沖刺激下,溝道電流呈現(xiàn)類似生物突觸的雙脈沖易化特性。人造突觸的短程塑性與雙電層靜電耦合調(diào)控有關(guān),而長(zhǎng)程塑性與溝道電化學(xué)摻雜有關(guān)。另外,基于突觸晶體管的雙柵和多柵工作模式,我們發(fā)現(xiàn)共平面的側(cè)柵之間可以相互調(diào)控、相互制約,并實(shí)現(xiàn)了兩個(gè)突觸輸入的雙脈沖易化和信息時(shí)空整合。通過改變調(diào)控柵極的輸入信號(hào)實(shí)現(xiàn)了“與”和“或”脈沖邏輯,以上工作為突觸電子學(xué)和神經(jīng)形態(tài)計(jì)算奠定了材料和器件基礎(chǔ)。(3)基于氧化物雙電層晶體管的多巴胺傳感器。采用PECVD法制備了具有高離子電導(dǎo)率的SiO_2質(zhì)子導(dǎo)體薄膜,發(fā)現(xiàn)薄膜具有較大的雙電層電容(~2.0μF/cm~2)。SiO_2質(zhì)子導(dǎo)體薄膜的疏松孔道中吸附的水分子對(duì)雙電層的形成起著關(guān)鍵的作用,質(zhì)子在薄膜內(nèi)部的傳導(dǎo)遵循格羅斯特機(jī)理。采用SiO_2質(zhì)子導(dǎo)體膜作為柵介質(zhì)層在導(dǎo)電玻璃襯底上研制了高性能低壓氧化物雙電層晶體管,待測(cè)溶液中的多巴胺分子與ITO柵極表面的苯硼酸特異性結(jié)合形成帶負(fù)電荷的多巴胺-硼酸酯絡(luò)合物,改變了柵極的表面電勢(shì)從而使晶體管的轉(zhuǎn)移曲線出現(xiàn)漂移。由此我們基于氧化物雙電層晶體管實(shí)現(xiàn)了多巴胺傳感,該多巴胺傳感器表現(xiàn)出較高的靈敏度和較好的選擇性。在低的工作電壓(0.8 V)下多巴胺的檢測(cè)極限低至0.1n M。
[Abstract]:In recent years, because of the huge double layer capacitance effect of electrolyte materials, the researchers have used electrolytes as the gate dielectric materials for transistors to achieve low voltage transistors. However, most of these transistors are based on liquid electrolyte grid media and organic semiconductors channel. There are some defects. The solid-state electrolyte is used as the gate dielectric material of the oxide thin film transistor, which reduces the working voltage of the device while having good structural expansibility and device stability. It also helps to design novel device structure. In addition, the unique ionic polarity response in the electrolyte and the very strong ion / ion at the interface of the device are also available. The electron coupling phenomenon is in line with the demand in the field of neural bionics and biochemical sensing. In this paper, the oxide double layer transistors, such as the sodium alginate proton conductor film, the self supporting chitosan proton conductor membrane and the SiO_2 proton conductor membrane, are studied in this paper. The main work of this paper can be summarized as follows: (1) the sodium alginate film is prepared by a simple coating method. It is found that the film has a larger double layer capacitance (~4.6 mu F/cm~2) and a high proton conductivity (~7.7 x 10-4 S/cm). The higher the temperature, the higher the relative humidity, the higher the relative humidity, the sodium alginate proton conductor The higher the double layer capacitance of the membrane, the proton conducting membrane of the sodium alginate proton conductors has three dimensional proton conduction characteristics, and the proton can migrate far away from the lateral electric field to form the lateral proton / electron coupling. We successfully developed the low pressure lateral coupled oxide double layer transistor with the sodium alginate proton conductor membrane for the first time. The current switch is ~3.1 x 106, the operating voltage is 1.5 V, the threshold voltage is -0.1 V, the saturation field effect mobility is 9.5 cm~2/V s, the sub threshold swing is 100 m V/dec., and the resistance load inverter based on the sodium alginate control side coupled oxide double layer transistor is developed. When the inverter's power supply voltage is 1 V, the voltage gain is high. Up to 5. is based on the dual gate operation mode of the side coupled oxide double layer transistor based on sodium alginate to realize the gate logic function. Finally, the sodium alginate proton conductor paper oxide double layer transistor is prepared on the flexible paper substrate, which shows good transistor performance under the lower working voltage and is based on both sides. The gate mode realizes the logic function with the gate. (2) the self supporting chitosan film is prepared by a simple coating and stripping process. It is found that the thin film has a large lateral double layer capacitance (~0.7 mu F/cm~2). The experimental results show that the self supported chitosan film is a solid electrolyte membrane with electronic insulation but proton conduction. We first use the self supporting shell. As the gate dielectric layer of the transistor, the self supported flexible oxide double layer transistor has been successfully developed. The current switching ratio of the self supporting flexible oxide double layer transistor is 106, the operating voltage is 1.6 V, the threshold voltage is -0.2 V, the mobility is 14.2 cm~2/V. S, the sub threshold swing is 120 m V/dec, and it has good stability and anti bending performance. Double layer crystal is good at the same time. As an ion / electronic hybrid transistor, the electrical properties of the transistors are affected by ion migration and the coupling of ion / electronic interfaces. The liquid environment in the organism is filled with various ions. The information transfer process in the nervous system is similar to that of the coupling phenomenon. Therefore, we will support the self supported flexible oxide double layer transistor as a self support. Artificial synapses have studied the memory / learning of the synaptic device, short range / long range plasticity, high pass filtering and multi input spatiotemporal information integration. Under the stimulation of the positive gate pressure pulse, the channel current is similar to the EPSC characteristic of the biological synapse; the channel current presents the dual pulse susceptibility to the biological synapse under the double pulse stimulation. The short range ductility of the contact is related to the electrostatic coupling of the electric double layer, while the long range plasticity is related to the channel electrochemical doping. In addition, based on the double gate and multi gate mode of the synaptic transistors, we find that the common plane grids can be controlled and restricted to each other, and two synaptic inputs are realized and the information space-time integration is realized. The "and" and "" pulse logic are realized by changing the input signal of the regulating gate. The above work lays the material and device basis for the synaptic electronics and the neural morphology calculation. (3) the dopamine sensor based on the oxide double layer transistor is used to prepare the SiO_2 proton conductor thin film with high ionic conductivity by PECVD. The present film has a large double layer capacitance (~2.0 mu F/cm~2).SiO_2 proton conductor film and the water molecules adsorbed in the porous channel play a key role in the formation of the double layer. The conduction of the proton in the film follows the grunst mechanism. The high performance of the SiO_2 proton conductor film is used as the gate dielectric layer on the conductive glass substrate. The low pressure oxide double layer transistor, the dopamine molecules in the solution to be specifically combined with the boric acid on the surface of the ITO gate to form a negatively charged dopamine borate complex, which changes the surface potential of the gate and thus leads to the shift of the transistor transfer curve. Thus, we have realized DOPA based on the oxide double layer transistor. Amine sensing showed that the dopamine sensor exhibited high sensitivity and selectivity. The detection limit of dopamine was as low as 0.1N M. at a low working voltage (0.8 V).

【學(xué)位授予單位】:中國科學(xué)院寧波材料技術(shù)與工程研究所
【學(xué)位級(jí)別】:博士
【學(xué)位授予年份】:2016
【分類號(hào)】:TN32

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