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《狄拉克半金属的能带调控和超快动力学研究（英文版）》利用超快时间分辨-角分辨光电子能谱系统对狄拉克半金属展开研究，揭示了狄拉克半金属Cd3As2中三维狄拉克费米子的能量、动量分辨的超快动力学过程，对此类拓扑量子材料的性质探究做出了贡献。
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| 內容簡介： |
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《狄拉克半金属的能带调控和超快动力学研究（英文版）》针对超快时间分辨角分辨光电子能谱系统的研制以及两个典型狄拉克半金属材料的电子能谱和超快动力学开展研究，取得了多项创新性研究成果。包括成功研制出光子能量连续可调的超快时间分辨角分辨光电子能谱系统，为研究三维量子材料的超快动力学提供了重要的实验手段；通过Li 插层形成凯库勒序石墨烯，首次提供了手征对称性破缺这一重要物理效应的直接实验证据；并观测到了增强的电子-声子耦合作用，以及与凯库勒序关联的平带电子结构；首次直接揭示了狄拉克半金属Cd3As2 中三维狄拉克费米子的能量、动量分辨的超快动力学过程，发现了长寿命的布居数反转效应。
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| 關於作者： |
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鲍昌华在清华大学物理系于2016年获得数学物理基础科学学士学位，2022年获得物理学博士学位，目前在水木清华学者计划资助下开展博士后研究，专注于利用先进角分辨光电子能谱仪研究二维和拓扑材料中的新奇电子结构和光-物质相互作用。
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| 目錄：
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1 Introduction 1
1.1 Overview of Dirac Semimetal 1
1.1.1 2D Dirac Semimetal 1
1.1.2 3D Dirac Semimetal 3
1.2 Intriguing Light-Matter Interaction in Dirac Semimetal 4
1.2.1 Ultrafast Dynamics and Population Inversion 4
1.2.2 Floquet Engineering in Dirac Semimetal 6
References 10
2 Experimental Techniques 15
2.1 Angle-Resolved Photoemission Spectroscopy 15
2.1.1 Basic Principles 15
2.1.2 Instruments 18
2.2 Time- and Angle-Resolved Photoemission Spectroscopy 20
2.2.1 Basic Principles 21
2.2.2 Special Technical Considerations 22
References 24
3 Development of Novel TrARPES with Tunable Probe Photon Energy for 3D Quantum Materials 27
3.1 Research Motivation 27
3.2 TrARPES with Tunable Probe Photon Energy 28
3.2.1 Experimental Setup 28
3.2.2 Tunable Probe Photon Energy 30
3.2.3 Considerations for the Time Resolution 33
3.2.4 TrARPES Functionality 39
3.3 Conclusions 40
References 40
4 Chiral Symmetry Breaking in Kekulé-Ordered Graphene 43
4.1 Research Motivation 43
4.2 Experimental Evidence of Chiral Symmetry Breaking 44
4.2.1 Preparation of Kekulé-Ordered Graphene 44
4.2.2 Evidence of CSB 1: Band Gap Opening 48
4.2.3 Evidence of CSB 2: Kekulé-O Order 50
4.2.4 Evidence of CSB 3: Chirality Mixing 51
4.3 Conclusion 55
References 55
5 Coexistence of Flat Band and Kekulé Order 59
5.1 Research Motivation 59
5.2 Extremely High Doping Level 60
5.3 Strong el-ph Coupling 62
5.4 Co-development of Flat Band and Kekulé Order 63
5.5 Conclusion 65
References 66
6 Dirac Fermion Cooling in 3D Dirac Semimetal Cd3As2 69
6.1 Research Motivation 69
6.2 Revealing the 3D Dirac Cone 70
6.3 Photoexcited Carrier Dynamics 71
6.4 Ultrafast Thermodynamics 73
6.5 Population Inversion 73
6.6 Conclusion 76
References 76
7 Summary and Prospects 79
References 80
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Dirac semimetals exhibit unique electronic band structure， novel physical properties with rich light-matter interaction， and potential applications. Revealing the band engineering and ultrafast dynamics of Dirac semimetals is therefore important. In this thesis， we develop the .rst time-and angle-resolved photoemission spectroscopy (TrARPES) with tunable probe photon energy and investigate the band structure engineering and ultrafast dynamics of Dirac semimetals by utilizing such a unique TrARPES system. Below are major scienti.c achievements:
(1)
We report the development of a TrARPES system with a highly tunable probe photon energy from 5.3 to 7.0 eV. Our TrARPES system has high energy， momentum， and time resolution (280–320 fs)， which opens up new opportunities for exploring ultrafast dynamics in 3D quantum materials.
(2)
We realize the long-sought-after chiral symmetry breaking (CSB) via Li inter-calation of graphene and provide direct experimental evidences. The CSB is evidenced by the gap opening at the Dirac point， Kekeulé-O type modulation， and chirality mixing near the gap edge. In addition， we also report the experi-mental observation of an extended .at band below EF in this system with strong electron-phonon interaction which coexists and codevelops with the Kekulé order， thus providing opportunities for investigating CSB-related physics， .at band-related instabilities， and its interplay with the Kekulé order.
(3)
We reveal the ultrafast dynamics of Dirac fermions in a model 3D Dirac semimetal Cd3As2 by using our TrARPES system with a tunable probe photon energy. The energy and momentum-resolved relaxation rate shows a linear dependence on the energy， suggesting Dirac fermion cooling through intraband relaxation. Moreover， a population inversion with a long lifetime of 3.0 ps is reported， which paves an important step toward exploring the possible dynamic exotic excitonic insulator.
This thesis advances the research of the electronic structure of Dirac semimetal from two aspects. First， it identi.es the Kekulé-ordered graphene as a new system for exploring chiral symmetry breaking-related physics including electronic frac-tionalization and topology effect and .at band-induced instability， including chiral
Abstract
superconductivity， especially providing a rare system to investigating their interplay. Secondly， this thesis solves the long-standing challenge of directly visualizing the non-equilibrium band structure of 3D Dirac semimetal and opens up new opportu-nities for exploring the light-matter interaction in 3D quantum materials， especially the light-induced topological phase transitions in 3D topological material through Floquet engineering.
Keywords Dirac semimetal · Band engineering · Ultrafast dynamics · Angle-resolved photoemission spectroscopy (ARPES) · Time-and angle-resolved photoe-mission spectroscopy (TrARPES)
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