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Interlayer Interaction in Graphene-Based Heterostructures

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Title
Interlayer Interaction in Graphene-Based Heterostructures
Alternative Title
그래핀 기반 헤테로 구조의 층간 상호작용
DGIST Authors
Soyun KimYoungwook KimChang-hee Cho
Advisor
김영욱
Co-Advisor(s)
Chang-hee Cho
Issued Date
2025
Awarded Date
2025-08-01
Type
Thesis
Description
Heterostructure, Proximity effect, Interlayer interaction, Spin-orbit coupling, Kitaev paramagnetic phase
Abstract

This thesis investigates proximity effects and interlayer interactions in van der Waals heterostructures composed of two-dimensional materials, focusing on graphene interfaced with various types of materials, including graphene itself, magnetic insulators and semimetals. Utilizing advanced fabrication techniques and systematic transport and spectroscopic measurements, the work explores how magnetic, electronic, and structural proximity can be tailored to engineer novel quantum phenomena. First, we demonstrate the formation of complex quantum Hall states in large-angle twisted bilayer graphene systems, where interlayer tunneling is suppressed, allowing access to ultra-strong Coulomb coupling regimes. We than examine 𝛼-RuCl3/bilayer graphene heterostructures, revealing spin-selective band hybridization and multiple Fermi surfaces. We further explore 𝛼-RuCl3/hBN/graphene heterostructures, where gate-induced hysteresis emerges below 50 K due to interfacial dipole alignment. The effect depends on hBN spacer thickness and shows no magnetic field dependence, suggesting a spin-lattice-dipole coupling linked to Kitaev paramagnetic fluctuations. Additionally, we evaluate the contact properties of Sb electrodes on 2D semiconductors such as MoS2, MoTe2, and WSe2. Low contact resistance and strong gate modulation are achieved. Carrier density enhancement via 𝛼-RuCl3 proximity in WSe2 heterostructures further highlights the utility of magnetic insulators as doping agents. Together, these results provide comprehensive insights into engineering interfacial coupling and proximity effects in 2D heterostructures, with implications for quantum electronic devices and next-generation contact technologies.|본 논문은 이차원 물질로 구성된 반 데르 발스 헤테로 구조에서의 근접 효과와 층간 상호작용에 대해 연구하였다. 특히 그래핀과 자기 절연체 또는 준금속 등을 포함한 다양한 소재 간의 계면 결합을 중심으로, 첨단 소자 제작 기법과 수송 및 분광 측정을 통해 자기적, 전자적, 구조적 근접 효과가 어떻게 새로운 양자 현상을 유도할 수 있는지를 체계적으로 탐구하였다.
먼저, 큰 비틀림 각을 갖는 이중층 그래핀에서의 양자 홀 상태 형성을 관측하였다. 이 시스템에서는 층간 터널링이 억제되어 강한 쿨롱 상호작용 영역에 접근할 수 있다. 이후, ⍺-RuCl3/이중층 그래핀 헤테로 구조에서는 스핀 선택적인 밴드 혼성화와 다수의 페르미 표면이 형성됨을 확인하였다. 이어서 ⍺-RuCl3/hBN/그래핀 구조를 연구하였고, 50 K 이하에서 계면 쌍극자의 정렬에 의해 발생하는 게이트 유도 히스테리시스를 관찰하였다. 이 효과는 hBN 스페이서 두께에 따라 달라지며, 자기장에는 영향을 받지 않아 키타에브 상자성체의 스핀격자-쌍극자 결합 가능성을 시사한다. 추가적으로, Sb 전극이 MoS2, MoTe2, WSe2 와 같은 이차원 반도체와 접촉할 때의 물성을 평가하였다. 낮은 접촉 저항과 우수한 게이트 조절 능력이 구현되었으며, ⍺-RuCl3 와의 근접 효과를 이용한 WSe2 의 캐리어 밀도 향상도 확인되어 자기 절연체가 도핑 소스로 활용될 수 있는 가능성도 제시하였다.
이러한 결과들은 이차원 헤테로 구조에서의 계면 결합과 근접 효과를 제어하는 전략에 대한 통합적인 통찰을 제공하며, 차세대 양자 전자소자 및 접촉 기술 개발에 기여할 수 있는 가능성을 시사한다.

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Table Of Contents
Ⅰ. Introduction 1
1.1 Two-Dimensional System 2
1.1.1 GaAs Quantum Wells 3
1.1.2 Graphene 4
1.2 Quantum Hall Effects 6
1.2.1 Classical Hall Effect 7
1.2.2 Quantum Oscillations 8
1.2.3 Integer Quantum Hall Effect 13
1.2.4 Fractional Quantum Hall Effect 17
1.3 Proximity Effect 20
1.3.1 Spin-Orbit Coupling 20
1.3.2 Magnetic Proximity Effect 23
ⅠⅠ. Quantum Hall States in Large Angle Twisted Double Bilayer Graphene 25
2.1 Introduction 25
2.1.1 Quantum Hall States in Graphene and Bilayer Graphene 25
2.1.2 Quantum Hall States in Double Layer System 28
2.1.3 Quantum Hall States in Large Angle Twisted Bilayer Graphene 32
2.2 Devices 36
2.3 Methods 36
2.4 Result and Discussion 37
2.4.1 Band Gap Opening 37
2.4.2 Integer Quantum Hall Effect 40
2.4.3 Fractional Quantum Hall Effect 45
2.5 Conclusion 49
2.6 Acknowledgements 49
IⅠⅠ. Proximity Effects in ⍺-RuCl3/Bilayer Graphene Heterostructure 50
3.1 Introduction 50
3.1.1 Characteristics of ⍺-RuCl3 50
3.1.2 Proximity Effects of ⍺-RuCl3/Graphene Heterostructure 53
3.2 Devices 55
3.2.1 Device Fabrication 55
3.2.2 Device for Lithium Intercalation 56
3.3 Methods 56
3.4 Results and Discussion 57
3.4.1 Transport Measurement 58
3.4.2 Theoretical Calculation 62
3.4.3 Effective Mass Calculation 66
3.4.4 Lithium Intercalation 69
3.5 Conclusion 72
3.6 Acknowledgements 72
3.7 Further Experiments 73
3.7.1 CrCl3/Monolayer Graphene Structure 73
3.7.2 CrCl3/Bilayer Graphene Structure 78
3.7.3 Conclusion 82
ⅠV. ⍺-RuCl3/thin BN/Graphene Heterostructure 83
4.1 Introduction 83
4.1.1 Interlayer Separation 83
4.2 Devices 84
4.3 Methods 85
4.4 Results and Discussion 87
4.4.1 Raman Spectroscopy 87
4.4.2 Transport Measurement 92
4.4 Conclusion 100
V. Ohmic Contact of 2D Semiconductor 101
5.1 Introduction 101
5.1.1 Proximity Induced Doping with 2D Material 101
5.1.2 Proximity Induced Band Hybridization with Semimetal 103
5.2 Devices 105
5.3 Results and Discussion 106
5.3.1 RuCl3/WSe2 Heterostructure 106
5.3.2 Sb Contact on 2D Semiconductors 108
5.4 Conclusion 115
5.5 Acknowledgements 115
References 116
URI
https://scholar.dgist.ac.kr/handle/20.500.11750/59802
http://dgist.dcollection.net/common/orgView/200000893020
DOI
10.22677/THESIS.200000893020
Degree
Doctor
Department
Department of Physics and Chemistry
Publisher
DGIST
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