单层膜图案诱导组装有机发光分子
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摘要
有机发光分子在发光二极管、平板显示器、光子器件等众多领域中得到了广泛的应用,越来越多的科研工作者投入到这方面的研究。由于制备大面积、高分辨率的有机功能材料图案对电子发光器件、信息存储、传感器、有机场效应晶体管等有着重要的意义,因此这是非常重要的一项研究。
本论文主要通过纳米压印技术制备单层膜图案,并以其作为模板诱导组装有机发光分子,研究内容如下:
1.我们借助纳米压印技术,在硅基底上制备氨基硅烷分子(APTMS)的自组装单层膜(SAM)图案,真空热蒸镀有机发光分子,研究了图案周期、温度和储存时间对分子沉积行为的影响。
2.我们在硅基底上借助纳米压印,不用经过真空气相沉积硅烷分子,直接制备了聚甲基丙烯酸甲酯(PMMA)聚合物单层膜结构,在其表面真空热蒸镀有机发光分子,并对其形貌、分子沉积的选择性进行了研究。
3.我们制备了三种单层膜:APTMS单层膜、氟取代硅烷化试剂(FDTS)单层膜、PMMA聚合物单层膜,对其形貌、分子沉积的选择性进行了对比研究。
本论文的创新性在于我们可以借助纳米压印技术,通过自组装不同性质的单分子薄膜,对基底进行表面修饰,使基底表面功能化,从而将有机发光分子组装到预期位置。这种方法提供了一种高效的制备大面积高分辨率有机发光分子图案的新途径。
Organic light emitting molecules have been widely used in the fields of light emitting diodes, displays and other optical devices due to their low cost and wide applicability,which has attracted intensive research interests. For the fabrication of integrated organic electronic devices, information storage, sensors, organic field-effect transistor, it is important to pattern organic materials over large areas with high resolution. Organic luminescent molecules are used in fabricating organic film via gas deposition. Micromachining Technology is firstly applied in fabricating organic luminescent molecules, and the conventional method for micropatterning small-molecule films is based on shadow mask technology. Unfortunately, this method has limitations in achieving high resolution because of shadow effects and presents difficulties in applying over a large area. Several alternative patterning methods have also been developed, such as photolithography, microcontact printing (μCP), organic vapor jet printing , cold welding, soft lithography, and nanosphere lithography, electron-beam lithography, ion-beam lithography and so on. As an emerging technique, nanoimprint lithography provides a way to fabricate low-cost, high-throughput, high-resolution pattern.
Besides the top-down fabrication methods, fabrication of organic light emitting molecules patterns based on bottom-up methods has received more and more attention. Templated assembly method is used in fabrication of organic material pattern gradually. Self-assembly monolayers (SAM) achieved great success in supramolecular assembly system. Organic silane molecules connect with the substrate by covalent bonding with high stability. Organic silane pattern make the surface functional. Template-directed growth of organic materials in gas phase can avoid ambient contamination (water and oxygen), and be readily compatible with matured semiconductor processing technology.
In this work, we used patterned self-assembled monolayer (SAM) fabricated by NIL as a template to direct the deposition of organic luminescent molecules .The study follows:
1. Based on nanoimprint lithography, APTMS SAM pattern was achieved on silicon substrate, which directed the deposition of organic luminescent molecules via gas phase deposition and studied the effect of morphology, molecule deposition, storage time, geometry of the pattern, and substrate temperature on the aggregation of organic luminescent molecules. Deposit organic luminescent molecules via gas phase deposition onto the SAM decorated Si substrate. At first molecules deposited on the sample surface disorderly, including the APTMS regions and substrate surface. With extending the storage time, the organic luminescent molecules move onto the APTMS monolayer from Si substrate and form a thin uniform organic film. I control the substrate temperature by heating the substrate in evaporation process. The amount of the molecules domain between the lines decreased and molecules move faster with the temperature increased, but the molecules domain between the APTMS lines became larger. At the same time, organic luminescent molecules can move onto the APTMS SAM. The distance that organic luminescent molecules can move is limited. In a certain time, the largest distance is fixed. The number of organic luminescent molecules that the APTMS SAM can contain is a certain value. The larger the SAM area is, the more molecules it can contain. Organic luminescent molecules can be deposited onto the APTMS SAM by fabricating APTMS pattern with proper geometry, achieving selective deposition of organic luminescent molecules. In this way, well-ordered organic luminescent molecules patterns were fabricated. Two kinds of substrate were chosen in the experiment and three kinds of organic luminescent molecules were selected, which achieved similar results. It proves that the method can be used with other different organic light emitting molecules. This versatile method provides a promising route for large area patterning of organic light emitting molecules with high resolution and high throughput.
2. PMMA monolayer was fabricated on silicon substrate via nanoimprint lithography without deposition of APTMS via gas phase deposition. Deposite organic luminescent molecules via gas phase deposition and do research into morphology and selective deposition of molecules. It was found that the experiment results when organic luminescent molecules deposited on the PMMA were similar with that of deposition onto the APTMS SAM. With increasing the time, molecules move to the PMMA monolayer. The distance molecules can move is limited and the number of molecules PMMA monolayer can contain is related to the area of monolayer. By fabricating PMMA pattern with proper geometry, selective deposition of organic luminescent molecules can be achieved with orderly organic luminescent molecules patterns fabricated.
3. Three kinds of monolayer were fabricated: APTMS, FDTS, PMMA monolayer. I made comparison on the morphology and selective deposition during the research. Deposite organic luminescent molecules via gas phase deposition on three kinds of monolayer with no structure. It is easier to form a uniform thin film on APTMS and PMMA monolayer, and form many organic domains on FDTS monolayer. We make different kinds of SAM pattern for compare the influence of different SAM to the organic molecules. We found FDTS monolayer had the lowest surface energy, so the molecules would deposite on the other monolayers, and the organic molecules prefer to deposite the APTMS monolayer, because of its highest surface energy.
In conclusion, a template-directed method for patterning organic light emitting molecules is demonstrated. Based on Nanoimprinting Lithography, the self-assembled monolayer pattern provides different surface energies, and induces organic light emitting molecules depositing on anticipated positions. This versatile method provides a promising route for large area patterning of organic light emitting molecules with high resolution and high throughput.
本论文主要通过纳米压印技术制备单层膜图案,并以其作为模板诱导组装有机发光分子,研究内容如下:
1.我们借助纳米压印技术,在硅基底上制备氨基硅烷分子(APTMS)的自组装单层膜(SAM)图案,真空热蒸镀有机发光分子,研究了图案周期、温度和储存时间对分子沉积行为的影响。
2.我们在硅基底上借助纳米压印,不用经过真空气相沉积硅烷分子,直接制备了聚甲基丙烯酸甲酯(PMMA)聚合物单层膜结构,在其表面真空热蒸镀有机发光分子,并对其形貌、分子沉积的选择性进行了研究。
3.我们制备了三种单层膜:APTMS单层膜、氟取代硅烷化试剂(FDTS)单层膜、PMMA聚合物单层膜,对其形貌、分子沉积的选择性进行了对比研究。
本论文的创新性在于我们可以借助纳米压印技术,通过自组装不同性质的单分子薄膜,对基底进行表面修饰,使基底表面功能化,从而将有机发光分子组装到预期位置。这种方法提供了一种高效的制备大面积高分辨率有机发光分子图案的新途径。
Organic light emitting molecules have been widely used in the fields of light emitting diodes, displays and other optical devices due to their low cost and wide applicability,which has attracted intensive research interests. For the fabrication of integrated organic electronic devices, information storage, sensors, organic field-effect transistor, it is important to pattern organic materials over large areas with high resolution. Organic luminescent molecules are used in fabricating organic film via gas deposition. Micromachining Technology is firstly applied in fabricating organic luminescent molecules, and the conventional method for micropatterning small-molecule films is based on shadow mask technology. Unfortunately, this method has limitations in achieving high resolution because of shadow effects and presents difficulties in applying over a large area. Several alternative patterning methods have also been developed, such as photolithography, microcontact printing (μCP), organic vapor jet printing , cold welding, soft lithography, and nanosphere lithography, electron-beam lithography, ion-beam lithography and so on. As an emerging technique, nanoimprint lithography provides a way to fabricate low-cost, high-throughput, high-resolution pattern.
Besides the top-down fabrication methods, fabrication of organic light emitting molecules patterns based on bottom-up methods has received more and more attention. Templated assembly method is used in fabrication of organic material pattern gradually. Self-assembly monolayers (SAM) achieved great success in supramolecular assembly system. Organic silane molecules connect with the substrate by covalent bonding with high stability. Organic silane pattern make the surface functional. Template-directed growth of organic materials in gas phase can avoid ambient contamination (water and oxygen), and be readily compatible with matured semiconductor processing technology.
In this work, we used patterned self-assembled monolayer (SAM) fabricated by NIL as a template to direct the deposition of organic luminescent molecules .The study follows:
1. Based on nanoimprint lithography, APTMS SAM pattern was achieved on silicon substrate, which directed the deposition of organic luminescent molecules via gas phase deposition and studied the effect of morphology, molecule deposition, storage time, geometry of the pattern, and substrate temperature on the aggregation of organic luminescent molecules. Deposit organic luminescent molecules via gas phase deposition onto the SAM decorated Si substrate. At first molecules deposited on the sample surface disorderly, including the APTMS regions and substrate surface. With extending the storage time, the organic luminescent molecules move onto the APTMS monolayer from Si substrate and form a thin uniform organic film. I control the substrate temperature by heating the substrate in evaporation process. The amount of the molecules domain between the lines decreased and molecules move faster with the temperature increased, but the molecules domain between the APTMS lines became larger. At the same time, organic luminescent molecules can move onto the APTMS SAM. The distance that organic luminescent molecules can move is limited. In a certain time, the largest distance is fixed. The number of organic luminescent molecules that the APTMS SAM can contain is a certain value. The larger the SAM area is, the more molecules it can contain. Organic luminescent molecules can be deposited onto the APTMS SAM by fabricating APTMS pattern with proper geometry, achieving selective deposition of organic luminescent molecules. In this way, well-ordered organic luminescent molecules patterns were fabricated. Two kinds of substrate were chosen in the experiment and three kinds of organic luminescent molecules were selected, which achieved similar results. It proves that the method can be used with other different organic light emitting molecules. This versatile method provides a promising route for large area patterning of organic light emitting molecules with high resolution and high throughput.
2. PMMA monolayer was fabricated on silicon substrate via nanoimprint lithography without deposition of APTMS via gas phase deposition. Deposite organic luminescent molecules via gas phase deposition and do research into morphology and selective deposition of molecules. It was found that the experiment results when organic luminescent molecules deposited on the PMMA were similar with that of deposition onto the APTMS SAM. With increasing the time, molecules move to the PMMA monolayer. The distance molecules can move is limited and the number of molecules PMMA monolayer can contain is related to the area of monolayer. By fabricating PMMA pattern with proper geometry, selective deposition of organic luminescent molecules can be achieved with orderly organic luminescent molecules patterns fabricated.
3. Three kinds of monolayer were fabricated: APTMS, FDTS, PMMA monolayer. I made comparison on the morphology and selective deposition during the research. Deposite organic luminescent molecules via gas phase deposition on three kinds of monolayer with no structure. It is easier to form a uniform thin film on APTMS and PMMA monolayer, and form many organic domains on FDTS monolayer. We make different kinds of SAM pattern for compare the influence of different SAM to the organic molecules. We found FDTS monolayer had the lowest surface energy, so the molecules would deposite on the other monolayers, and the organic molecules prefer to deposite the APTMS monolayer, because of its highest surface energy.
In conclusion, a template-directed method for patterning organic light emitting molecules is demonstrated. Based on Nanoimprinting Lithography, the self-assembled monolayer pattern provides different surface energies, and induces organic light emitting molecules depositing on anticipated positions. This versatile method provides a promising route for large area patterning of organic light emitting molecules with high resolution and high throughput.
引文
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[2] FORREST S R. The path to ubiquitous and low-cost organic electronic appliances on plastic [J]. Nature, 2004, 428(6986): 911-918.
[3] SHEN Z, BURROWS P E, BULOVIC V, et al. Three-color, tunable, organic light-emitting devices [J]. Science, 1997, 276: 2009-2011.
[4] TIAN P F, BULOVIC V, BURROWS P E, et al. Precise, scalable shadow mask patterning of vacuum-deposited organic light emitting devices [J]. Journal of Vacuum Science & Technology a-Vacuum Surfaces and Films, 1999, 17(5): 2975-2981.
[5] RAKOW N A, SUSLICK K S. A colorimetric sensor array for odour visualization [J]. Nature, 2000, 406(6797): 710-713.
[6] BURROWS P E, WILSON E G. The inchworm memory-a new molecular electronic device [J]. Journal of Molecular Electronics, 1990, 6(4): 209-220.
[7] BULOVIC V, DESHPANDE R, THOMPSON M E, et al. Tuning the color emission of thin film molecular organic light emitting devices by the solid state solvation effect [J]. Chemical Physics Letters, 1999, (308): 317.
[8]陈志强. Oled有机发光二极体显示器技术[M].台北县:全华图书股份有限公司2007.
[9]闫东航,王海波,杜宝勋.有机半导体异质结导论[M].北京:科学出版社, 2008.
[10]张红雨.酚基吡啶硼发光配合物:多晶相及发光性能研究[D].长春:吉林大学化学学院, 2006.
[34] EDMAN L, RIGLER R. Memory landscapes of single-enzyme molecules [J]. Proceedings of the National Academy of Sciences of the United States of America, 2000, 97(15): 8266-8271.
[35] MOLLER S, PERLOV C, JACKSON W, et al. A polymer/semiconductor write-once read-many-times memory [J]. Nature, 2003, 426(6963): 166-169.
[36] RAMANATHAN K, BANGAR M A, YUN M H, et al. Individually addressable conducting polymer nanowires array [J]. Nano Letters, 2004, 4(7): 1237-1239.
[37] CUI Y, WEI Q Q, PARK H K, et al. Nanowire nanosensors for highly sensitive and selective detection of biological and chemical species [J]. Science, 2001, 293(5533): 1289-1292.
[38] KONG J, FRANKLIN N R, ZHOU C W, et al. Nanotube molecular wires as chemical sensors [J]. Science, 2000, 287(5453): 622-625.
[39] FREUND M S, LEWIS N S. A chemically diverse conducting polymer-based“electronic nose”[J]. Proceedings of the National Academy of Sciences of the United States of America, 1995, 92: 2652-2656.
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