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研究生：	陳敬岡 Chen, Ching-Kang
論文名稱：	量子點應用於雞蛋白薄膜電晶體記憶元件之研究 Investigation of Albumen Thin Film Transistor Memories Using Quantum Dots
指導教授：	蘇炎坤 Su, Yan-Kuin
學位類別：	碩士 Master
系所名稱：	電機資訊學院 - 微電子工程研究所 Institute of Microelectronics
論文出版年：	2013
畢業學年度：	101
語文別：	英文
論文頁數：	81
中文關鍵詞：	微接觸壓印、有機記憶電晶體、並五苯、量子點、雞蛋白、水
外文關鍵詞：	microcontact printing, organic memory thin film transistor, pentacene, quantum dots, chicken albumen, water
相關次數：	點閱：117 下載：2
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本論文中，主要探討運用微接觸壓印技術沉積量子點(QDs)薄膜於有機薄膜電晶體記憶元件之研究。在有機薄膜電晶體研究中，由於此壓印方式可有效減少有機溶劑對於薄膜品質上之破壞，另外相較於傳統旋轉塗佈方式，此壓印方式更具有薄膜圖案化的優勢，因此將此壓印技術運用於元件製成中，可有效減少漏電流路徑。在本研究中的壓印方式上，運用聚二甲基矽氧烷(PDMS)製作出壓印所需要的印章，將量子點均勻旋轉塗佈於PDMS印章上，隨後壓印於介電層材料上，其量子點可作為記憶體元件中之浮動閘極，達成臨界電壓值的改變以實現記憶體效果。
在量子點於電晶體式記憶體應用方面，我們採用n+型矽(閘極電極)/氧化矽(介電層)/聚甲基丙烯酸甲酯(黏貼層)/量子點(浮動閘極)/並五苯(通道層)/金(源極及汲極層)為基本結構。傳統元件中利用量子點與聚甲基丙烯酸甲酯混合溶液在旋轉塗佈後形成浮動閘極之薄膜;有別於此方式，我們運用聚二甲基矽氧烷印章成功將量子點轉印至聚甲基丙烯酸甲酯之上，量子點在元件中扮演抓取載子的重要角色。此元件於電性量測上可進行電晶體操作，記憶體操作上，記憶儲存窗在磁滯測試中可由原本傳統旋轉塗佈方式量子點(QDs)記憶電晶體的25 V提高到74.3 V，開關操作上可以達到一百次，並在一百次操作後仍然能辨別出 ”1” 和 “0”的邏輯分別，保存時間上可以達到32年 (109秒)的效果。
在雞蛋白電晶體和記憶電晶體研究方面，在前半段運用水於雞蛋白薄膜表面旋轉塗佈以達到改變表面自由能，將雞蛋白表面自由能提高至與主動層(並五苯)相匹配後，可發現並五苯結晶品質獲得顯著地改善。由於主動層並五苯結晶品質會直接影響到電晶體之特性，運用水處理過後，雞蛋白電晶體良率由原本12.5%提升至80%。後半部實驗則是運用壓印方式將量子點轉印在雞蛋白薄膜之上，傳統旋轉塗佈方式在原子力顯微鏡(AFM)量測下雞蛋薄膜表面粗糙度為3.48 nm，而在運用壓印方式下，表面粗糙度降低至2.48 nm; 為了更為有效降低表面粗糙度，在雞蛋白薄膜上利用水進行表面處理，雞蛋白在水的保護下可免於被甲苯溶劑所破壞，表面粗糙度更降為1.47 nm，壓印量子點後成功製作出量子點浮動閘極，以獲得雞蛋白記憶電晶體效果，記憶儲存窗可達到50.33 V，但在開關特性和穩定度測試中，此雞蛋白介電層記憶元件能有待改善的空間。

The main purpose of this thesis was focused on the deposition of quantum dots (QDs) thin film in organic memory thin film transistors by microcontact printing technique. In the study of organic thin film transistors, the transfer contact printing method could effectively prevent the destruction of thin film from organic solvent. Besides, contact printing technique has the advantage of thin film patterning. Therefore, the number of leakage current paths could be effectively reduced by the application of contact printing technique in the fabricated procedures. In this study, we used polydimethylsiloxane (PDMS) to be the stamps. After spin coating the QDs on the PDMS stamp, the QDs were then transferred onto the dielectric layer subsequently. The QDs can be used as floating gate of the devices. Floating gate partially offset the internal electric field which inducing the shift of threshold voltage. The shift of threshold voltage accomplished memory effect.
In the study of QDs’ application for transistor-type memory, the basic structure was n+ - Si (gate electrode)/SiO2 (dielectric layer)/poly(methyl methacrylate) (PMMA) (adhesion layer)/quantum dots (floating gate)/pentacene (channel layer)/gold (source and drain layer). The floating gate of conventional devices was fabricated by spin coating the QD-PMMA composite on the SiO2 thin film. Compared with spin coating method, using the PDMS stamp can also successfully transfer QDs onto PMMA layer. The QDs were playing in an important role to capture the carrier charges in the transistor device. The device showed typical transistor characteristics under electrical operation. Under hysteresis testing, the memory window could increase from 25 V with spin coating method to 74.3 V using contact printing technique. And the switching property exhibited over 100 write-read-erase-read cycles. Furthermore, the retention time achieved more than 32 years (109 seconds).
In study of albumen based thin film transistors and memory transistors, the dielectric material was changed to be albumen which is friendly to our environment. The first half of experiment was spin-coating above the surface of chicken albumen thin film with water for changing surface free energy. After increasing the surface free energy of albumen thin film to match with that of active layer (pentacene film), the quality of pentacene crystal was markedly improved. Because the crystal quality of pentacene layer can directly affect performance of transistor, the yield rate could increase from 12.5% to 80% after water treatment. In last half of experiment, the contact printing method was used to fabricate quantum dots. Under Atomic Force Microscopy (AFM) measurements, the surface roughness of albumen film with spin coating method was 3.48 nm and could reduce to 2.48 nm by applying contact printing technique. Furthermore, the surface of chicken albumen thin film was treated by spin coating water for preventing the damage from toluene and efficiently reducing surface roughness. The surface roughness of albumen film could reach 1.47 nm with water protection. After transferring QDs onto albumen film, the transistor-type memory purpose was realized. In this device testing, the memory window was 50.33 V. But the switching property and stability of memory thin film transistors still have room to be improved.

Abstract (in Chinese) ……………………………………………………………………I
Abstract (in Engilsh) ……………………………………………………………………III
Acknowledgement……………………………………………………………………….Ⅵ
Content…………………………………….………………………………………...……Ⅶ
Table Captions …………………………….……………………………………………..Ⅹ
Figure Captions…………………………….…………………………………………….XI

Chapter 1 Introduction 
	1-1 The review of organic based memory devices (OMDs) ………………………1
1-2 Transistor-type memory ………………………………………………………...1
1-3 Floating gate organic thin film transistors ….……………………..………….2
Chapter 2 Principles of Floating Gate Organic Memory Thin-Film Transistor……8
2-1 Floating gate organic memory thin film transistors operation………….……8
2-2 Important parameters of organic memory thin film transistors…..………….9
   2-2.1 Field Effect Mobility….……………………….…………………………...9
2-2.2 Threshold Voltage.........…….……………….………...………………….10
2-2.3 Sub-threshold Slope ……………………………………………………...11
2-2.4 On/Off Current Ratio (ION/OFF).………………………………………….11
2-2.5 Memory Window (Threshold Voltage Shift)…..………..……………….11
2-2.6 Switching Property……………………………………………………….12
2-2.7 Retention Time……………………………………………………………12
	2-3 The Fabrication Methods of Floating gate…………………………….....…12


Chapter 3 Using Contact-Printing Method to Fabricate QDs as Floating Gate of Pentacene Based Organic Memory Thin Film Transistors…..………........19
	3-1 Motivation……………………………………………………………………...19
3-2 Performance Improvement of Nonvolatile Memory Thin Film Transistors with PMMA layer as decorating film .......................................……………….20
3-2.1 Experimental Details..………………………….………………………...20
	3-2.2 Results and Discussion…………………………. ……………………...21
3-3 Using contact-printing method to fabricate QDs as floating gate of pentacene based organic memory thin film transistor…………………….……………..22
3-3.1 Experimental Details..………………………….………………………...22
	3-3.2 Results and Discussion…………………………. ……………………...23
3-4 Using Double-Insulator layer to improve the QDs OTFTs performance……26
3-5 Summary…………………………………………………………………………26
Chapter 4 The Improvement of Albumen Dielectric Thin Film Transistors and   Fabrication of  Quantum Dots by Contact Printing Technique as Floating Gate in Albumen Memory Thin Film Transistors...................................................…………………………..........47
	4-1 Introduction…………………………………………………………………..…47
4-2 The Improvement of Organic Thin Film Transistors by Water Treatment on       
    the Surface of Albumen Dielectric Layer ………………...…..….….....…...48
	   4-2.1 Experimental Details………………………….………………………...48
	   4-2.2 Results and Discussion…………………………. ……………………...49
4-3 Using Contact-Printing Method to Fabricate Quantum Dots as Floating Gate 
in Albumen Memory Thin Film Transistors…………..………………..…..…52
       4-3.1 Experimental Details………………………….………………………...52
	   4-3.2 Results and Discussion……………...……………. ……………………...53
    4-4 Summary….…………………………………………………………………..…56
Chapter 5 Conclusions and Future Prospect…………………………………………...72
	5-1 Conclusions……………………………………………………………………...72
	5-2 Future Prospect…………………………………………………………………74
Reference …………………………………………………………………………………76


















Table Captions
Table 3-1. The important parameters of OTFTs………………………………………33
Table 3-2. 5 seconds contact printing and the substrate with room temperature     
          showed better uniformity…………………………………………………...36
Table 3-3. The important parameters of Device B and Device C……………………...40
Table 3-4. The comparison of memory window and charge carrier density………….42
Table 4-1. Comparison of surface free energy between pentacene film and albumen   
          surface…………….…………………….……………..…………………….60
Table 4-2. Comparison of pentacene film, albumen surface and albumen treated with     
         water.…………………..……………………………..…………………..……63
Table 4-3. The important parameters of transistor under drain-source voltage (VDS)    
          at -30 V operation…………………………………………….......…………66













Figure Captions
Figure 1-1 The statistics of publications and citations on organic/polymer memory during 1970~2013………………….………………………………………….4
Figure 1-2 Schematic view of (a) resistor-type, (b) capacitor-type and (c) transistor-type memory structure……………………………………………5
Figure 1-3 Schematic view of (a) bottom and (b) top contact OTFTs…………………6
Figure 1-4 The structure of the conventional floating gate memory…………………..7
Figure 2-1 The operation modes of OTFTs…………………………………………….15
Figure 2-2 Energy-band diagrams of floating gate operation with (a) zero, (b) positive VGS, and (c) negative VGS, respectively …………………………16
Figure 2-3 Typical electrical behaviors for organic memory thin film transistor……17
Figure 2-4 A variety of floating gate fabrication methods……………………………..18
Figure 3-1 (a) the pattern method of OLED; (b) RGB organic light emitting diode...28
Figure 3-2 The device structure of nonvolatile floating gate memory TFTs using surface decorating PMMA layer…………………………………………….29
Figure 3-3 Transmission Electron Microscopy (TEM) image of the QDs…………….30
Figure 3-4 The CCD camera images of sample’s surface (a) Device A (b) Device B…31
Figure 3-5 (a) Device A showed resistor characteristics; (b) Device B showed typical transistor property………………………...…………………………………32
Figure 3-6 Hysteresis measurement of QDs organic memory thin film transistors with PMMA decorating layer……………………………………………………..33
Figure 3-7 The new design procedures of contact printing method…………………..34
Figure 3-8 Fabrication process of PDMS stamp and organic memory thin film transistors……………………………………………………………………..40
Figure 3-9 Spin rate (a) of 500 rpm; (b) of 1000 rpm to prepare QDs on PDMS stamp………………………………………………………………………….37
Figure 3-10 The surface of sample (a) Device A, (b) Device B and (c) Device C…….38
Figure 3-11 The pentacene crystal quality increase from (a) to (c)…………………...39
Figure 3-12 Transfer characteristics of (a) Device B and (b) Device C as VGS swept from +Vmax to -Vmax and reverse. The VDS was fixed at -30 V……………40
Figure 3-13 Threshold voltage of (a) Device B and (b) Device C with “ON” and “OFF” state………………………………………………………………………….41
Figure 3-14 Write-Read-Erase-Read (WRER) cycles. (a) The writing signal was 200 V for 3s, erasing signal was -200 V for 3s and reading at 20 V for 3s. (b) After 100 times operation, the “ON” and “OFF” state still can be distinguished………………………………………………………………...42
Figure 3-15 Retention time property measurement. The ON/OFF ratio 
decreased to half after 5 × 105 seconds and totally loss the 
charges 109 seconds later…………………………………………………...43
Figure 3-16 The thin nylon 6 layer was deposited after QDs contact printing. The thickness of nylon 6 was 0.5 nm…………………………………………....44
Figure 3-17 Vmax was set at 60 V under VDS of -30 V…………………………………..45
Figure 3-18 The write voltage was 100 V, erase voltage was -100 V and read at -40 V for 5 seconds each…………………………………………………………..46
Figure 4-1 The albumen dielectric thin film transistor fabricating process. 
The Device B was treated with water above albumen film and 
Device A kept in original condition………………………………………….57
Figure 4-2 The transfer and output characteristics of Device A………………………58

Figure 4-3 The surface morphologies of the (a) pentacene and (b) albumen thin film of the device measured by Atomic Force Microscopy (AFM)…….………59
Figure 4-4 The contact angels of Device A were (a) 103.48° with water and (b) 50.75° with diiodomethane (MI) measurement…………………………………….60
Figure 4-5 The albumen surface morphologies after spin coating (a) toluene, 
(b) chloroform, (c) methyl alcohol and (d) water. The roughness were 
3.48 nm, 4.17 nm, 3.97 nm and 1.27 nm, respectively……………………...61
Figure 4-6 The FTIR spectrum almost overlapped together………………………….62
Figure 4-7 The contact angle of Device B measured with (a) water and 
(b) Diiodomethane (MI) 〖CH〗_2 I_2……………………………………………..63
Figure 4-8 Compared with Fig 4-3 (a), the pentacene crystal quality was more smooth and better……………………………………………………………………..64
Figure 4-9 The capacitance of albumen layers of Device A and Device B with drive frequency of 1000 (1 k) Hz at sweeping voltage from – 20 V to 20 V……..64
Figure 4-10 The electric characteristics in Device B was improved (a) transfer property (b) output of transistor…………………………………………...65
Figure 4-11 The details about quantum dots floating gate albumen dielectric 
memory TFTs fabrication process…………………………………………67
Figure 4-12 The (a) and (c) showed albumen surfaces of Device A and Device B after contact printing with toluene; (b) and (d) were the surface morphologies after contact printing quantum dots at Device A and Device B………….68
Figure 4-13 The output and transfer properties of Device A were shown in (a) and (b); (c) and (d) for Device B……………………………………………………..69
Figure 4-14 Transfer characteristics of Device B as VGS were swept from +Vmax to -Vmax, and turned back then. The amplitude of Vmax was varied from 20 to 80 V, which VDS was fixed at -40 V…………………………………………70
Figure 4-15 Switching (write-read-erase-read) cycles. 
The bias parameters of programming, erasing and reading were 
VGS = +80 V, -55 V and -80 V.........................................................................71
Figure 4-16 The stability test. The transfer and hysteresis properties were 
measured again after 60 days. The drain-source voltage (VGS) was 
fixed at -30 V………………………………………………………………...72

                                    

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校內：2020-07-01公開
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