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Optical Spectroscopy of Two Dimensional Graphene and Boron Nitride


This dissertation describes the use of optical spectroscopy in studying the physical properties of two dimensional nano materials like graphene and hexagonal boron nitride. Compared to bulk materials, atomically thin two dimensional materials have a unique character that is the strong dependence of physical properties on external control. Both electronic band structure and chemical potential can be tuned in situ by electric field-which is a powerful knob in experiment. Therefore the optical study at atomic thickness scale can greatly benefit from modern micro-fabrication technique and electric control of the material properties. As will be shown in this dissertation, such control of both gemometric and physical properties enables new possibilities of optical spectroscopic measurement as well as opto-electronic studies. Other experimental techniques like electric transport and scanning tunneling microscopy and spectroscopy are also combined with optical spectroscopy to reveal the physics that is beyond the reach of each individual technique.

There are three major themes in the dissertation. The first one is focused on the study of

plasmon excitation of Dirac electrons in monolayer graphene. Unlike plasmons in ordinary two dimensional electron gas, plasmons of 2D electrons as in graphene obey unusual scaling laws. We fabricate graphene micro-ribbon arrays with photolithography technique and use optical absorption spectroscopy to study its absorption spectrum. The experimental result demonstrates the extraordinarily strong light-plasmon coupling and its novel dependence on both charge doping and geometric dimensions. This work provides a first glance at the fundamental properties of graphene plasmons and forms the basis of an emerging subfield of graphene research and applications such as graphene terahertz metamaterials.

The second part describes the opto-electronic response of heterostructures composed of

graphene and hexagonal boron nitride. We found that there is a charge transfer process

between graphene and BN when the exposure of visible light is introduced. We show this photo-induced doping in graphene resembles the modulation doping technique in traditional semiconductor heterojunctions, where a charge doping is introduced while the high mobility is maintained. This work reveals importance of interactions between stacked 2D materials on the overall properties and demonstrate a repeatable and convenient way of fabricating high quality graphene devices with active control of doping patterning. Along this direction, we did further STM experiment to visualize and manipulate charged defects in boron nitride with the help of graphene.

The last theme is about the interesting properties of bilayer graphene, which is to some

extent more interesting than monolayer graphene due to its electric-eld dependent band

structures. Firstly, we visualized the stacking boundary within exfoliated bilayer graphene by near field infrared microscopy. In dual-gated field-effect-transistor devices fabricated on the boundaries, we demonstrated the existence of topologically protected one dimensional conducting channels at the boundary through electric transport measurement. The 1D boundary states also demonstrated the first graphene-based valleytronic device.

The topics we are going to talk about in this thesis are quite diversified. Just like the

versatile nature of optical spectroscopy, we never limit ourself to a specific technique and

do incremental things. Most of the experiments are driven by the important and interesting problems in the two dimensional materials field and we chose the right tool and conceive the right experiment to answer that question. Both pure optical methods and combinations with electric transport and STM measurements were used. I believe the flexibility of optical spectroscopy and its compatibility with other experimental techniques provide a powerful toolbox to explore many possibilities beyond the reach of a single experimental approach. And such a way of doing experiments is very much enjoyable for me.

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