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      Effect of Polymer Architectures on the Self-Assembly Behaviors of Block Copolymers

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      https://www.riss.kr/link?id=T16653072

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      국문 초록 (Abstract) kakao i 다국어 번역

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      4차 산업혁명에 따른 전자제품 수요 증가 추세는 전 세계적으로 진행되고 있다.1 지난 몇년간, 전자제품에 대한 급증한 수요는 반도체 부족으로 이어졌다. 메모리 반도체와 로직 칩 분야에서는 소수의 반도체 기업만이 살아남았고 회사들은 현재 대형 실리콘 웨이퍼에서 누가 가장 작고 결함이 없는 패턴을 얻을 수 있는지를 두고 경쟁하고 있다. 지금까지의 반도체 생산에는 포토리소그래피 사용되어졌다. 그러나, 포토리소그래피는 조사된 빛의 파장으로 인해 분해능 한계를 갖는다는 점에서 한계가 있다. 이러한 본질적인 단점과 높은 비용의 부담을 극복하기 위해 과학자들과 엔지니어들은 대안적인 해결책을 찾게 되었다. 블록공중합체 리소그래피는 기존 포토리소그래피가 가지고 있는 단점을 모두 커버할 수 있는 솔루션을 제공한다.

      블록공중합체 리소그래피는 칩을 제조하기 위한 나노패턴의 제조에 있어서 대체가능한 기술로서 각광받고 있다.2-4 블록공중합체 (BCP)는 2개 이상의 화학적으로 구별되는 블록이 공유결합된 고분자의 종류이다. 블록공중합체는 많은 제어/리빙 중합 기술을 사용하여 실험실에서 쉽게 합성될 수 있다. 블록 공중합체는 유리 전이 온도(Tg) 이상에서 어닐링을 하게 되면 다양한 나노 패턴을 형성할 수 있다.2-4 이러한 특성으로 인해 지난 수십 년 동안 선형 블록 공중합체에 대한 연구가 널리 연구되어 왔다. 선형 블록 공중합체를 사용하여 형성된 나노구조체는 다음과 같은 특성을 갖는다: (i) 5~70 nm의 도메인 크기를 갖는다. (ii) 라멜라, 실린더, 자이로이드, 스피어를 포함한 다양한 모폴로지가 구현될 수 있다. (iii) 다양한 고분자 재료를 사용하여 다양한 기능기를 제공할 수 있다. (iv) 저비용 및 광범위한 가용성 등 고분자 재료의 통상적인 장점을 가지고 있다. 이에 따라 포토리소그래피의 대안으로 10nm 이하의 나노구조를 만들기 위한 광범위한 연구가 진행되고 있다.

      논문의 첫 부분에서, 블록공중합체의 상분리를 촉진하기 위한 새로운 접근법을 소개하였다. 특이 구조인 스타 구조 블록공중합체가 합성되었고 아키텍쳐 특성상 묶인 구조로 인해 선형 블록공중합체에 비한 엔트로피의 감소가 발생하여 자체 조립 거동이 촉진된다. 음이온 중합을 바탕으로 스타 PS-b-PLA 블록공중합체가 합성되었고, 상분리 현상을 유사한 분자량 및 부피 분율을 갖는 선형 PS-b-PLA 블록공중합체와 비교하였다. 분석 기법들을 이용하여 도메인 크기의 감소와 함께 선형 블록 공중합체에 비해 스타 블록 공중합체의 상분리 촉진 거동이 보고되었다.

      블록공중합체 리소그래피가 산업에 적용되기 위해서는 박막상에서 수직 배향을 유도하고, 박막상에서 자기조립하면서 발생하는 불가피한 결함 등 극복해야 할 몇 가지 마일스톤들이 존재한다. 논문의 두 번째 부분은 표면 중화제로서의 병솔형 고분자의 응용에 대해 다루고 있다. 랜덤 공중합체 곁사슬을 갖는 병솔형 고분자를 합성하여 기존 PS-b-PMMA 및 높은 χ값을 가지는 PS-b-PMAA 선형 블록 공중합체의 표면 중화제로 사용하였다. 선형 블록공중합체와 병솔형 고분자를 혼합하고 스핀코팅을 진행하게 되면 엔트로픽적 효과로 인해 병솔형 고분자가 블록공중합체 박막의 공기와의 계면과 기판 계면을 향해 분리되도록 하였다. 랜덤공중합체 곁사슬의 비율은 샌드위치된 선형 블록 공중합체에 대한 중립 조건으로 작용하도록 세심하게 제어되어 수직 방향의 라멜라 형태로 구현을 가능케 하였다.

      진행 중인 프로젝트 및 전망 섹션에서는 논문의 두번째 부분에서 소개한 개념에 대한 후속 연구와 100nm 이상의 나노패턴을 형성할 수 있는 병솔형 블록 공중합체에 대한 연구에 대한 진행상황을 소개하였다.
      번역하기

      4차 산업혁명에 따른 전자제품 수요 증가 추세는 전 세계적으로 진행되고 있다.1 지난 몇년간, 전자제품에 대한 급증한 수요는 반도체 부족으로 이어졌다. 메모리 반도체와 로직 칩 분야에서...

      4차 산업혁명에 따른 전자제품 수요 증가 추세는 전 세계적으로 진행되고 있다.1 지난 몇년간, 전자제품에 대한 급증한 수요는 반도체 부족으로 이어졌다. 메모리 반도체와 로직 칩 분야에서는 소수의 반도체 기업만이 살아남았고 회사들은 현재 대형 실리콘 웨이퍼에서 누가 가장 작고 결함이 없는 패턴을 얻을 수 있는지를 두고 경쟁하고 있다. 지금까지의 반도체 생산에는 포토리소그래피 사용되어졌다. 그러나, 포토리소그래피는 조사된 빛의 파장으로 인해 분해능 한계를 갖는다는 점에서 한계가 있다. 이러한 본질적인 단점과 높은 비용의 부담을 극복하기 위해 과학자들과 엔지니어들은 대안적인 해결책을 찾게 되었다. 블록공중합체 리소그래피는 기존 포토리소그래피가 가지고 있는 단점을 모두 커버할 수 있는 솔루션을 제공한다.

      블록공중합체 리소그래피는 칩을 제조하기 위한 나노패턴의 제조에 있어서 대체가능한 기술로서 각광받고 있다.2-4 블록공중합체 (BCP)는 2개 이상의 화학적으로 구별되는 블록이 공유결합된 고분자의 종류이다. 블록공중합체는 많은 제어/리빙 중합 기술을 사용하여 실험실에서 쉽게 합성될 수 있다. 블록 공중합체는 유리 전이 온도(Tg) 이상에서 어닐링을 하게 되면 다양한 나노 패턴을 형성할 수 있다.2-4 이러한 특성으로 인해 지난 수십 년 동안 선형 블록 공중합체에 대한 연구가 널리 연구되어 왔다. 선형 블록 공중합체를 사용하여 형성된 나노구조체는 다음과 같은 특성을 갖는다: (i) 5~70 nm의 도메인 크기를 갖는다. (ii) 라멜라, 실린더, 자이로이드, 스피어를 포함한 다양한 모폴로지가 구현될 수 있다. (iii) 다양한 고분자 재료를 사용하여 다양한 기능기를 제공할 수 있다. (iv) 저비용 및 광범위한 가용성 등 고분자 재료의 통상적인 장점을 가지고 있다. 이에 따라 포토리소그래피의 대안으로 10nm 이하의 나노구조를 만들기 위한 광범위한 연구가 진행되고 있다.

      논문의 첫 부분에서, 블록공중합체의 상분리를 촉진하기 위한 새로운 접근법을 소개하였다. 특이 구조인 스타 구조 블록공중합체가 합성되었고 아키텍쳐 특성상 묶인 구조로 인해 선형 블록공중합체에 비한 엔트로피의 감소가 발생하여 자체 조립 거동이 촉진된다. 음이온 중합을 바탕으로 스타 PS-b-PLA 블록공중합체가 합성되었고, 상분리 현상을 유사한 분자량 및 부피 분율을 갖는 선형 PS-b-PLA 블록공중합체와 비교하였다. 분석 기법들을 이용하여 도메인 크기의 감소와 함께 선형 블록 공중합체에 비해 스타 블록 공중합체의 상분리 촉진 거동이 보고되었다.

      블록공중합체 리소그래피가 산업에 적용되기 위해서는 박막상에서 수직 배향을 유도하고, 박막상에서 자기조립하면서 발생하는 불가피한 결함 등 극복해야 할 몇 가지 마일스톤들이 존재한다. 논문의 두 번째 부분은 표면 중화제로서의 병솔형 고분자의 응용에 대해 다루고 있다. 랜덤 공중합체 곁사슬을 갖는 병솔형 고분자를 합성하여 기존 PS-b-PMMA 및 높은 χ값을 가지는 PS-b-PMAA 선형 블록 공중합체의 표면 중화제로 사용하였다. 선형 블록공중합체와 병솔형 고분자를 혼합하고 스핀코팅을 진행하게 되면 엔트로픽적 효과로 인해 병솔형 고분자가 블록공중합체 박막의 공기와의 계면과 기판 계면을 향해 분리되도록 하였다. 랜덤공중합체 곁사슬의 비율은 샌드위치된 선형 블록 공중합체에 대한 중립 조건으로 작용하도록 세심하게 제어되어 수직 방향의 라멜라 형태로 구현을 가능케 하였다.

      진행 중인 프로젝트 및 전망 섹션에서는 논문의 두번째 부분에서 소개한 개념에 대한 후속 연구와 100nm 이상의 나노패턴을 형성할 수 있는 병솔형 블록 공중합체에 대한 연구에 대한 진행상황을 소개하였다.

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      다국어 초록 (Multilingual Abstract) kakao i 다국어 번역

      영어
      한국어
      Growing tide of demand for electronics in accordance with the 4th industrial revolution has been an ongoing trend worldwide.1 During the last decade, this rocketed demand for electronics led to shortage of semiconductors. In the field of memory semiconductors and logic chips, only a handful of semiconductor companies have survived. The remaining companies are currently competing for who can get the smallest, defectless pattern on large silicon wafers. So far, photolithography has been used for semiconductor production. However, due to wavelength of the irradiated light, conventional photolithography is limited in that it has resolution limit. This in turn sets a boundary in how low the half-pitch can reach which is usually around 10-20 nm. To overcome this inherent downside, and the burden of high cost have led scientists and engineers to look for alternative solutions. Block copolymer lithography offers a solution that can cover all the downsides that conventional photolithography lithography has.
      Block copolymer lithography has been in the spotlight as the replaceable technology in producing nano-patterns for manufacturing chips.2-4 Block copolymer (BCP) is a type of polymer with two or more chemically distinct blocks covalently bonded to each other. BCP can easily be synthesized in lab using many controlled/living polymerization techniques. Block copolymers can form various nanopatterns when heated above glass transition temperature (Tg).2-4 Due to this characteristic, studies into linear block copolymers have been widely researched in the past few decades. The nanostructures formed using linear block copolymers has following properties: (i) Feature sizes ranging from 5 to 70 nm. (ii) A variety of morphologies, including lamellar, cylinders, gyroids, spheres can be created. (iii) Various polymer materials can be used to provide functionality and qualities. (iv) It possesses the conventional benefits of polymeric materials, such as low cost and widespread availability. As a result, extensive research has been conducted to create sub-10 nm nano-structures as an alternative to photolithography.
      In the first part of the dissertation, we demonstrate a novel approach to promote the phase separation of block copolymers. Block copolymer of unique star architecture has been synthesized and due to the existing conjunction in polymer architecture, decrease in translational entropy occurs, leading to a promotion in self-assembly behavior. Synthesis of well-defined miktoarm PS-b-PLA BCPs have been done and compared their segregation behaviors with those of linear PS-b-PLA BCPs having similar molecular weights and volume fraction. Using various analytical techniques, phase promotion behaviors of miktoarm block copolymers compared to linear block copolymers along with decreased domain sizes have been reported.
      For block copolymer lithography to be applied in industry, there are some obstacles to overcome such as inducing perpendicular orientation on thin film and the inevitable defects that occur while being self-assembled on thin film. The second part of the dissertation covers implementing bottlebrush polymer as surface neutralizer. Bottlebrush polymers having random copolymer side chains were synthesized to be used as surface neutralizers for conventional PS-b-PMMA and high-χ PS-b-PMAA linear block copolymers. When bottlebrush polymers were blended with linear block copolymers, bottlebrush polymer’s high chain end to mid monomer ratio led to entropic effect of bottlebrush polymers to segregate towards the bottom and top surface of block copolymer thin films. The random copolymer side chain ratios were carefully controlled to act as a neutral condition to the linear block copolymers, leading to perpendicularly oriented lamellar morphologies.
      In the ongoing and outlook section, follow-up study of the concepts introduced in the second part of the dissertation as well as study of bottlebrush block copolymers that can form supra-100nm nanopatterns are reported.
      번역하기

      Growing tide of demand for electronics in accordance with the 4th industrial revolution has been an ongoing trend worldwide.1 During the last decade, this rocketed demand for electronics led to shortage of semiconductors. In the field of memory semico...

      Growing tide of demand for electronics in accordance with the 4th industrial revolution has been an ongoing trend worldwide.1 During the last decade, this rocketed demand for electronics led to shortage of semiconductors. In the field of memory semiconductors and logic chips, only a handful of semiconductor companies have survived. The remaining companies are currently competing for who can get the smallest, defectless pattern on large silicon wafers. So far, photolithography has been used for semiconductor production. However, due to wavelength of the irradiated light, conventional photolithography is limited in that it has resolution limit. This in turn sets a boundary in how low the half-pitch can reach which is usually around 10-20 nm. To overcome this inherent downside, and the burden of high cost have led scientists and engineers to look for alternative solutions. Block copolymer lithography offers a solution that can cover all the downsides that conventional photolithography lithography has.
      Block copolymer lithography has been in the spotlight as the replaceable technology in producing nano-patterns for manufacturing chips.2-4 Block copolymer (BCP) is a type of polymer with two or more chemically distinct blocks covalently bonded to each other. BCP can easily be synthesized in lab using many controlled/living polymerization techniques. Block copolymers can form various nanopatterns when heated above glass transition temperature (Tg).2-4 Due to this characteristic, studies into linear block copolymers have been widely researched in the past few decades. The nanostructures formed using linear block copolymers has following properties: (i) Feature sizes ranging from 5 to 70 nm. (ii) A variety of morphologies, including lamellar, cylinders, gyroids, spheres can be created. (iii) Various polymer materials can be used to provide functionality and qualities. (iv) It possesses the conventional benefits of polymeric materials, such as low cost and widespread availability. As a result, extensive research has been conducted to create sub-10 nm nano-structures as an alternative to photolithography.
      In the first part of the dissertation, we demonstrate a novel approach to promote the phase separation of block copolymers. Block copolymer of unique star architecture has been synthesized and due to the existing conjunction in polymer architecture, decrease in translational entropy occurs, leading to a promotion in self-assembly behavior. Synthesis of well-defined miktoarm PS-b-PLA BCPs have been done and compared their segregation behaviors with those of linear PS-b-PLA BCPs having similar molecular weights and volume fraction. Using various analytical techniques, phase promotion behaviors of miktoarm block copolymers compared to linear block copolymers along with decreased domain sizes have been reported.
      For block copolymer lithography to be applied in industry, there are some obstacles to overcome such as inducing perpendicular orientation on thin film and the inevitable defects that occur while being self-assembled on thin film. The second part of the dissertation covers implementing bottlebrush polymer as surface neutralizer. Bottlebrush polymers having random copolymer side chains were synthesized to be used as surface neutralizers for conventional PS-b-PMMA and high-χ PS-b-PMAA linear block copolymers. When bottlebrush polymers were blended with linear block copolymers, bottlebrush polymer’s high chain end to mid monomer ratio led to entropic effect of bottlebrush polymers to segregate towards the bottom and top surface of block copolymer thin films. The random copolymer side chain ratios were carefully controlled to act as a neutral condition to the linear block copolymers, leading to perpendicularly oriented lamellar morphologies.
      In the ongoing and outlook section, follow-up study of the concepts introduced in the second part of the dissertation as well as study of bottlebrush block copolymers that can form supra-100nm nanopatterns are reported.

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      목차 (Table of Contents)

      • CHAPTER 1. INTRODUCTION 1
      • 1.1 Block Copolymers 1
      • 1.1.1 Phase Separation of Block Copolymers 1
      • 1.1.2 Approaches for Perpendicular Orientation of Block Copolymers 9
      • 1.2 Bottlebrush Polymers 12
      • CHAPTER 1. INTRODUCTION 1
      • 1.1 Block Copolymers 1
      • 1.1.1 Phase Separation of Block Copolymers 1
      • 1.1.2 Approaches for Perpendicular Orientation of Block Copolymers 9
      • 1.2 Bottlebrush Polymers 12
      • 1.2.1 Fundamentals of Bottlebrush Polymers 12
      • 1.2.2 Synthesis and characterization of BBCPs 14
      • 1.3 References 19
      • CHAPTER 2. The Effect of Chain Architecture on the Phase Behavior of A4B4 Miktoarm Block Copolymers 38
      • 2.1 Introduction 38
      • 2.1.1 Abstract 38
      • 2.1.2 Miktoarm Polymers: Simulation Results 39
      • 2.1.3 Miktoarm Polymers: Previous Works and This Study 41
      • 2.2 Experimental Methods 43
      • 2.3 Characterization 71
      • 2.4 Results and Discussion 73
      • 2.5 Conclusions 80
      • 2.6 References 81
      • CHAPTER 3. Bottlebrush Copolymer as Surface Neutralizer for Vertical Alignment of Block Copolymer Nanodomains in Thin Films 86
      • 3.1 Introduction 86
      • 3.1.1 Abstract 86
      • 3.1.2 Top-Coat Approach 88
      • 3.1.3 Polymer Additive Approach 89
      • 3.1.4 Scope of Bottlebrush Additive Research 91
      • 3.2 Experimental Methods 96
      • 3.3 Results and Discussions 122
      • 3.4 Conclusions 135
      • 3.5 References 136
      • CHAPTER 4. Ongoing Research and Outlook 141
      • 4.1 Ongoing Research 141
      • 4.2 Bottlebrush Copolymer as Surface Neutralizer for Vertical Alignment of Hydrophobic Block Copolymer System 143
      • 4.2.1 Experimental Methods 143
      • 4.2.2 Results and Discussion 150
      • 4.3 Synthesis of Bottlebrush Block Copolymer and Alignment of Supra-100 nm Pattern 153
      • 4.3.1 Experimental Methods 153
      • 4.3.2 Results and Discussion 166
      • 4.4 References 167
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      참고문헌 (Reference)

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      83. Hierarchical Photonic Pigments via the Confined Self-Assembly of Bottlebrush Block Copolymers, Guidetti, G., Zhao, T. H., Parker, R. M., Song, D. P., Vignolini, S., 13, 1764-1771, , 2019

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