臺灣博碩士論文加值系統

在本論文中，吾人研製了一系列的肖特基接觸式氫氣感測器。藉由觸媒金屬(鈀或鉑)作為閘極金屬，氫氣分子會被解離成氫原子；同時部分的氫原子將會擴散通過觸媒金屬層並吸附在金屬-氧化層或金屬-半導體的介面；最後這些氫原子會被極化成一偶極層。此一偶極層的存在將會改變肖特基接觸式氫氣感測器之電流-電壓特性。實驗得知，肖特基接觸式氫氣感測器具備低氫氣濃度之探測能力、耐高溫以及寬廣的操作範圍。此外，短暫的響應時間亦是此氫氣感測器之優點。
首先，吾人製作了以磷化銦鋁為主動層，鉑金屬-氧化層-半導體及鉑金屬-半導體肖特基二極體式氫氣感測器。不論是在順偏壓或者是逆偏壓，此元件皆具有寬廣的溫度操作範圍和高氫氣探測能力，並且能夠探測很低含量的氫氣濃度(4.3 ppm H2/air)。同時，針對氧化層的存在與否作探討，發現具有氧化層之元件，其介面能夠吸附較多的氫原子，獲得較高的感測靈敏度。此外，對於氣體動力機制亦有深入的研究與探討。
接著，為了研究載氣對氫氣感測之影響，製作了鉑金屬-氧化層-氮化鎵肖特基式氫氣感測器。在以合成空氣為載氣及包含9970 ppm氫氣的環境下，其串聯電阻由191.8 Ω降低到155.3 Ω。然而，以高純度氮氣取代合成空氣為載氣並且導入4.3 ppm的氫氣時，得到較為顯著的開通電壓和串聯電阻變化量，其分別為0.32 V和19.56 Ω。推斷合成空氣中的氧氣將會和氫氣反應形成氫氧基及水，導致較少的氫原子進入觸媒金屬。此外，即使在室溫下，此一元件依然能夠快速地感測到氫氣的存在。
為了加強所轉換出的電子訊號，並且增加實用價值，吾人進一步研製了具有電氣訊號放大功能的擬晶性高電子移動率電晶體，作為氫氣感測器。由實驗結果得知，此元件確實大幅度的提升了對氫氣的偵測能力。此外，藉由ISE模擬軟體，成功地描繪出擬晶性高電子移動率電晶體之電特性及其氫氣感測特性。
然後，吾人探究不同半導體材料之肖特基接觸對氫氣感測的影響，發現缺少磷化銦鎵層的元件，具有較好的氫氣感測能力，然其對溫度之穩定性較差。另一方面，藉由高純度氮氣為載氣的環境中，解析氫氣感測暫態響應之行為。
最後，吾人設計並製作一個具有放大功能的積體電路，其中包括 解碼器、傳輸閘極開關以及運算放大器三種電子元件。解碼器的運用提供了數個輸入閘，可同時接上數個感測器，產生數個不同的輸入訊號。電路的運作主要是將每個解碼器的輸出連結到開關的時脈輸入，來控制開關的開通與斷路，使得其中一個感測器的訊號能夠被導入運算放大器，最後得到一個放大的輸出訊號。除了可以同時控制數比輸入訊號，對於偵測低氫氣濃度亦具有極大的優勢。

In this dissertation, a series of Schottky contact-type hydrogen sensors are proposed. By using the catalytic metals (Pd or Pt) as the gate materials, the hydrogen molecules will be dissolved as hydrogen atoms. Part of those hydrogen atoms will diffuse through the metal bulk and adsorb at the metal-oxide or metal-semiconductor interface. Those adsorbed hydrogen atoms will be polarized to form a dipolar layer. Due to the presence of this dipolar layer, the significant changes in current-voltage characteristics of the studied devices are found. Experimentally, the studied hydrogen sensors can work in a low hydrogen concentration, high operating temperature, and wide hydrogen concentration range environments. Also, a short response time is observed in real-time applications. These results demonstrate the promise of the studied devices to perform as fast-responsive and sensitive hydrogen sensors over a broad range of operating temperature.
In chapter 2, the Pt-InAlP metal-oxide-semiconductor and metal-semiconductor Schottky diode hydrogen sensors with high-sensitive hydrogen detection among wide operating temperature regime are comprehensively studied and compared. Experimentally, both the hydrogen sensors can be operated systematically under bi-polarity biases. In addition, it is worth to note that even an extremely low hydrogen concentration of 4.3 ppm H2/air can be effectively detected at the temperature of 30~250oC. The detecting sensitivity of the MOS-type hydrogen sensor is superior to that of the MS-type. It is believed that a high-quality oxide layer effectively increases the amount of hydrogen atoms adsorbed. Also, the hydrogen effects are found on both the Schottky barrier height lowering and the modulation in the electric field at the Pt-oxide and Pt-InAlP interfaces.
In chapter 3, hydrogen sensing properties of a Pt-oxide-GaN metal-oxide-semiconductor-type Schottky diode is demonstrated and studied. In the hydrogen-containing environment, the shift of current-voltage curves and decrease of turn-on voltage Von are found to be caused by the lowering of Schottky barrier height. Also, the corresponding series resistance Rs is decreased from 191.8 (in air) to 155.3 Ω (under a 9970 ppm H2/air gas) at 30oC. As the carrier gas is replaced by a nitrogen gas, a significant variation of 0.32 V and 19.56 Ω in Von and Rs values are obtained at 30oC, respectively, even at an extremely low hydrogen concentration of 4.3 ppm H2/N2. Since the oxygen atoms will be dissolved on the Pt metal surface and react with hydrogen atoms by the formation of hydroxyl and water, the amount of adsorbed hydrogen atoms on the Pt surface is reduced. Moreover, the shorter response time constant and the larger initial rate of current density variation are found even at room temperature.
In chapter 4, an interesting transistor-type hydrogen sensing detector based on GaAs pseudomorphic high electron mobility transistor with a Pd/Al0.24Ga0.76As metal-semiconductor Schottky gate structure is fabricated and investigated. The significant modulations in electrical signals are observed obviously due to the adsorption of hydrogen atoms at Pd-semiconductor interface. The corresponding adsorption and desorption time constants (�跾 and �踀) are 2.5 and 6 sec, respectively, under a 9970 ppm H2/air gas at 160oC. Theoretically, the dipolar layer formed by the hydrogen atoms adsorbed at the Pd-AlGaAs interface can be considered as a two-dimensional layer. The simulated curves show excellent agreement with experimental results. In addition, an anomalous decrease phenomenon in transient response is observed, which may be caused by the formation of hydroxyl species and water. Consequentially, the studied device provides the promise for GaAs integrated circuit and micro electric and mechanic system applications.
In chapter 5, the interesting hydrogen sensing characteristics of two transistors with an Al0.24Ga0.76As (device A) and In0.49Ga0.51P (device B) Schottky layer are demonstrated. Experimentally, device A shows a lower hydrogen detection limit of 4.3 ppm H2/air, a higher current variation of 7.79 mA and a shorter adsorption time of 10.95 s in a 9970 ppm H2/air at room temperature. On the other hand, device B exhibits more stable hydrogen-sensing characteristics at high temperatures. In addition, the transient hydrogen sensing phenomenon of device A is studied. In an N2 environment, the sensing signal is proportion to the logarithmic values of hydrogen concentration at temperature from 30 to 160oC. Due to the higher activation energy for initiating the reverse hydrogen release process, the current-response of hydrogen-detecting signal is always not recovered back to the original baseline level. At higher temperature, the recovering curve can be divided into three regions: (i) initial, (ii) accumulation, and (iii) revival stages. Because the recombination process of hydrogen atoms is slower, larger amount of desorbed hydrogen atoms are accumulated on the Pd metal surface which results in the longer desorption time. However, the higher speed desorption phenomenon is observed in the presence of oxygen.
In chapter 6, a back-end amplifying integrated circuit is designed and fabricated. The output amplifying circuit is composed of three electronic devices including the decoder, CMOS transmission gate switch, and operational amplifier. Several input sensing signals can be introduced simultaneously and controlled by the decoder and switch. One of these input sensing signals can pass through the switch, and the output signal of the sensing signal is amplified.

Abstract
Table Captions
Figure Captions
Chapter 1 Introduction
1.1 Introduction........................................................................................................... 1
1.2 Gas Detection Apparatus and Measurement......................................................... 3
1.3 Disertations Organization...................................................................................... 4
Chapter 2 Comprehensive Investigation of Hydrogen-Sensing Properties of Pt/InAlP-Based Schottky Diodes
2.1 Introduction........................................................................................................... 6
2.2 Experimental........................................................................................................ 7
2.3 Results and Discussion......................................................................................... 8
2.4 Summary...............................................................................................................15
Chapter 3 Hydrogen-Sensing Properties of a Pt-oxide-GaN Schottky Diode
3.1 Introduction..........................................................................................................16
3.2 Experimental........................................................................................................17
3.3 Results and Discussion.........................................................................................18
3.4 Summary...............................................................................................................23
Chapter 4 Comprehensive Study of Hydrogen Sensing Properties of a Pd/Al0.24Ga0.76As-Based High Electron Mobility Transistor
4.1 Introduction..........................................................................................................24
4.2 Experimental........................................................................................................26

4.3 Results and Discussion.........................................................................................26
4.3.1 Steady-State Analysis...............................................................……………26
4.3.2 Transient-Response Analysis..................................................……………31
4.3.3 Simulation Analysis..................................................................……………34
4.4 Summary...............................................................................................................36
Chapter 5 Comprehensive Study of Pd-gate Metal-Oxide-Semiconductor Transistor-type Hydrogen Sensors
5.1 Introduction..........................................................................................................38
5.2 Experimental........................................................................................................40
5.3 Comparative Study of Hydrogen Sensing Characteristics of Pd-MOS Transistors with Al0.24Ga0.76As and In0.49Ga0.51P Schottky Contact Layers
5.3.1 Results and Discussion.............................................................……………41
5.3.2 Summary...................................................................................……………45
5.4 Transient Response of Hydrogen Sensing Phenomenon of a Pd-InGaP MOS-type Field-Effec Transistor
5.4.1 Results and Discussion.............................................................……………46
5.4.2 Summary...................................................................................……………50
5.5 Summary...............................................................................................................50
Chapter 6 Integration of Back-end Amplification Circuit
6.1 Introduction..........................................................................................................51
6.2 Experimental and Simulation...............................................................................53
6.3 Summary...............................................................................................................56

Chapter 7 Conclusion and Prospect
7.1 Conclusions.....................................................................................................….57
7.2 Prospects…….......................................................................................................58
References
Tables
Figures
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