The graphitic systems have attracted intensive attention recently due to the discovery of graphene, a single layer of graphite. The low-energy band structure of graphene exhibits an unusual linear dispersion relation which hosts massless Dirac fermions and leads to intriguing electronic and optical properties. In particular, due to the high mobility and tunability, graphene and graphitic materials have been recognized as promising candidates for future nanoelectronics and optoelectronics. Electron-phonon coupling (EPC) plays a significant role in electronic and optoelectronic devices. Therefore, it is crucial to understand EPC in graphitic materials and then manipulate it to achieve better device performance. In the first part of this thesis, we explore EPC between Dirac-like fermions and infrared active phonons in graphite via infrared magneto-spectroscopy. We demonstrate that the EPC can be tuned by varying the magnetic field. The second part of this thesis deals with magnetoplasmons in quasineutral graphene nanoribbons. Multilayer epitaxial graphene grown on the carbon terminated silicon carbide surface behaves like single layer graphene. Plasmons are excited in the nanoribbons of undoped multilayer epitaxial graphene. In a magnetic field, the cyclotron resonance can couple with the plasmon resonance forming the so-called upperhybrid mode. This mode exhibits a distinct dispersion relation, radically different from that expected for conventional two dimensional systems.

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京都大学 / 0048 / 新制・課程博士 / 博士(エネルギー科学) / 甲第22709号 / エネ博第406号 / 新制||エネ||78(附属図書館) / 京都大学大学院エネルギー科学研究科エネルギー基礎科学専攻 / (主査)教授 坂口 浩司, 教授 松田 一成, 教授 野平 俊之 / 学位規則第4条第1項該当 / Doctor of Energy Science / Kyoto University / DFAM

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Various solution-processed methods have been employed in this work. For the synthesis of graphene, a chemical exfoliation method has been used to generate large graphene flakes in the solution phase. In addition, chemical or electro polymerization has been used for synthesizing polyanthracene, which tends to form graphene nanoribbon through cyclodehydrogenation. For the device fabrication, graphene oxide (GO) thin films were deposited from solution phase on the vapor-silanzed aminosilane surface to make semiconducting active layer or conducting electrodes. Gold nanoparticles (AuNPs) were selectively self-assembled from solution phase to pattern nanowires.

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There is a compelling need to explore different material options as well as device structures to facilitate smooth transistor scaling for higher speed, higher density and lower power. The enormous potential of nanoelectronics, and nanotechnology in general, offers us the possibility of designing devices with added functionality. However, at the same time, the new materials come with their own challenges that need to be overcome. In this work, we have addressed some of these challenges in the context of quasi-2D Silicon, III-V semiconductor and graphene. Bulk Si is the most widely used semiconductor with an indirect bandgap of about 1.1 eV. However, when Si is thinned down to sub-10nm regime, the quasi-2D nature of the system changes the electronic properties of the material significantly due to the strong geometrical confinement. Using a tight-binding study, we show that in addition to the increase in bandgap due to quantization, it is possible to transform the original in direct bandgap to a direct one. The effective masses at different valleys are also shown to vary uniquely in an anisotropic way. This ultra-thin Si, when used as a channel in a double gate MOSFET structure, creates so called “volume in version” which is extensively investigated in this work. It has been found that the both the quantum confinement as well as the gating effect play a significant role in determining the spatial distribution of the charge, which in turn has an important role in the characteristics of transistor. Compound III-V semiconductors, like Inx Ga1-xAs, provide low effective mass and low density of states. This, when coupled with strong confinement in a nanowire channel transistor, leads to the “Ultimate Quantum Capacitance Limit” (UQCL) regime of operation, where only the lowest subband is occupied. In this regime, the channel capacitance is much smaller than the oxide capacitance and hence dominates in the total gate capacitance. It is found that the gate capacitance change qualitatively in the UQCL regime, allowing multi-peak, non-monotonic capacitance-voltage characteristics. It is also shown that in an ideal condition, UQCL provides improved current saturation, on-off ratio and energy-delay product, but a degraded intrinsic gate delay. UQCL shows better immunity towards series resistance effect due to increased channel resistance, but is more prone to interfacial traps. A careful design can provide a better on-off ratio at a given gate delay in UQCL compared to conventional MOSFET scenario. To achieve the full advantages of both FinFET and HEMT in III-V domain, a hybrid structure, called “HFinFET” is proposed which provides excellent on performance like HEMT with good gate control like FinFET. During on state, the carriers in the channel are provided using a delta-doped layer(like HEMT) from the top of a fin-like non-planar channel, and during off state, the gates along the side of the fin(like FinFET) help to pull-off the carriers from the channel. Using an effective mass based coupled Poisson-Schrodinger simulation, the proposed structure is found to outperform the state of the art planar and non-planar MOSFETs. By careful optimization of the gate to source-drain underlap, it is shown that the design window of the device can be increased to meet ITRS projections at similar gate length. In addition, the performance degradation of HFinFET in presence of interface traps has been found to be significantly mitigated by tuning the underlap parameter. Graphene is a popular 2D hexagonal carbon crystal with extraordinary electronic, mechani-cal and chemical properties. However, the zero band gap of grapheme has limited its application in digital electronics. One could create a bandgap in grapheme by making quasi-1D strips, called nanoribbon. However, the bandgap of these nanoribbons depends on the the type of the edge, depending on which, one can obtain either semiconducting or metallic nanoribbon. It has been shown that by the application of an external transverse field along the sides of a nanoribbon, one could not only modulate the magnitude of the bandgap, but also change it from direct to indirect. This could open up interesting possibilities for novel electronic and optoelectronic applications. The asymmetric potential distribution inside the nanoribbon is found to result in such direct to indirect bandgap transition. The corresponding carrier masses are also found to be modulated by the external field, following a transition from a“slow”electron to a“fast” electron and vice-versa. Experimentally, it is difficult to control the bandgap in nanoribbons as precise edge control at nanometer scale is nontrivial. One could also open a bandgap in a bilayer graphene, by the application of vertical electric field, which has raised a lot of interest for digital applications. Using a self-consistent tight binding theory, it is found that, inspite of this bandgap opening, the intrinsic bias dependent electronic structure and the screening effect limit the subthreshold slope of a metal source drain bilayer grapheme transistor at a relatively higher value-much above the Boltzmann limit. This in turn reduces the on-off ratio of the transistor significantly. To overcome this poor on-off ratio problem, a semiconductor source-drain structure has been proposed, where the minority carrier injection from the drain is largely switched off due to the bandgap of the drain. Using a self-consistent Non-Equilibrium Green’s Function(NEGF) approach, the proposed device is found to be extremely promising providing unipolar grapheme devices with large on-off ratio, improved subthreshold slope and better current saturation. At high drain bias, the transport properties of grapheme is extremely intriguing with a number of nontrivial effects. Optical phonons in monolayer grapheme couple with carriers in a much stronger way as compared to a bilayer due to selection rules. However, it is difficult to experimentally probe this through transport measurements in substrate supported grapheme as the surface polar phonons with typical low activation energy dominates the total scattering. However, at large drain field, the carriers obtain sufficient energy to interact with the optical phonons, and create so called ‘hot phonons’ which we have experimentally found to result in a negative differential conductance(NDC). The magnitude of this NDC is found to be much stronger in monolayer than in bilayer, which agrees with theoretical calculations. This NDC has also been shown to be compensated by extra minority carrier injection from drain at large bias resulting in an excellent current saturation through a fundamentally different mechanism as compared to velocity saturation. A transport model has been proposed based on the theory, and the experimental observations are found to be in agreement with the model.

This thesis describes the conductivity fluctuations or noise measurements in graphenebased field effect transistors. The main motivation was to study the effect of disorder on the electronic transport in graphene. In chapter 4, we report the noise measurements in graphene field effect (GraFET) transistors with varying layer numbers. We found that the density dependence of noise behaves oppositely for single and multilayer graphene. An analytical model has been proposed to understand the microscopic mechanism of noise in GraFETs, which reveals that noise is intimately connected to the band structure of graphene. Our results outline a simple portable method to separate the single layer devices from multi layered ones. Chapter 5 discusses the noise measurements in two systems with a bandgap: biased bilayer graphene and graphene nanoribbon. We show that noise is sensitive to the presence of a bandgap and becomes minimum when the bandgap is zero. At low temperature, mesoscopic graphene devices exhibit universal conductance fluctuations (UCF) arising due to quantum interference effect. In chapter 6, we have studied UCF in single layer graphene and show that it can be sensitive to the presence of various physical symmetries. We report that time reversal symmetry exists in graphene at low temperature and, for the first time, we observed enhanced UCF at lower carrier density where the scattering is dominated by the long-range Coulomb scattering. Chapter 7 presents the transport and noise measurements in single layer graphene in the quantum Hall regime. At ultra-low temperature several broken symmetry states appear in the lowest Landau level, which originate possibly due to strong electron-electron interactions. Our preliminary noise measurements in the quantum Hall regime reveal that the noise is sensitive to the bulk to edge transport and can be a powerful tool to investigate these new quantum states.

Diese Arbeit untersucht die Auswirkungen von Kantendefekten auf die Leitfähigkeit von Graphen-Nanobändern (GNRs). Es werden die Kantenatome von zigzag- und armchair-GNRs zufällig umverteilt. Mittels Tight-Binding-Verfahren und rekursivem Greenfunktions-Formalismus werden die Transmissionsspektren der Systeme berechnet und mit Landauer-Formalismus die Leitfähigkeit bei variierter Länge bestimmt. Aus der Leitfähigkeit in Abhängigkeit von der Länge wird die Lokalisierungslänge nach Anderson ermittelt. Es wurde berechnet, dass die Lokalisierungslänge bei rauhen zigzag-GNRs gegen einen konstanten Wert strebt. Bei armchair-GNRs wurde ein linearer Abfall der Lokalisierungslänge bei zunehmender Rauheit vorgefunden.:1. Einleitung 2. Physikalische Grundlagen 2.1 Graphen 2.2 Landauer-Formalismus 2.3 Tight-Binding-Verfahren 2.4 Greenfunktions-Formalismus 2.5 Anderson-Lokalisierung 3. Methoden 3.1 Bandstrukturen 3.2 Strukturerzeugung 3.2.1 Allgemeines 3.2.2 zigzag-GNRs 3.2.3 armchair-GNRs 3.3 Rauheitsparameter 3.4 Leitfähigkeit 3.5 Lokalisierungslänge 4. Ergebnisse 4.1 Atomumverteilung 4.2 Transmissionsspektren 4.3 Leitfähigkeit 4.4 Lokalisierungslängen 4.5 Weitere Rauheitsmaße 5. Zusammenfassung und Ausblick

The precise introduction of nonplanar pores in the backbone of graphene nanoribbon represents a great challenge. Here, we explore a synthetic strategy toward the preparation of nonplanar porous graphene nanoribbon from a predesigned dibromohexabenzotetracene monomer bearing four cove-edges. Successive thermal annealing steps of the monomers indicate that the dehalogenative aryl-aryl homocoupling yields a twisted polymer precursor on a gold surface and the subsequent cyclodehydrogenation leads to a defective porous graphene nanoribbon containing nonplanar [14]annulene pores and five-membered rings as characterized by scanning tunneling microscopy and noncontact atomic force microscopy. Although the C–C bonds producing [14] annulene pores are not achieved with high yield, our results provide new synthetic perspectives for the on-surface growth of nonplanar porous graphene nanoribbons.