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Title Page

Dedication

Curriculum Vitae

Contents

List of Publications 19

Abstract 21

Chapter 1. Introduction 24

1.1. Low-Dimensional Electronic Systems 25

1.1.1. Technological Perspective: Scaling Limit of Devices 25

1.1.2. Fundamental Perspective: Interesting Quantum Phenomena 27

1.1.3. Conventional Low-Dimensional Materials 31

1.2. Low-Dimensional Systems on Silicon Surfaces 34

1.2.1. Surface Reconstructions 34

1.2.2. Surface States as 1D and 2D electron gases 39

1.2.3. Technical Advantage of Surface Systems 42

1.3. Phase Transitions in Surface Systems 43

1.3.1. Indium Nanowires on Si(111) 43

1.3.2. Gold Nanowires on Stepped Si(111) 46

1.3.3. Silicide Nanowires on Silicon Surfaces 48

1.4. Pb Overlayers & Nanowires on Silicon Surfaces 49

1.4.1. Pb Overlayers on Flat Si(111) 49

1.4.2. Pb Nanowires on Stepped Si(111) 53

1.5. Scope & Organization of this Thesis 57

Chapter 2. Photoelectron Spectroscopy 60

2.1. Brief History 61

2.2. Principle of ARPES 65

2.2.1. Energy Conservation 66

2.2.2. Momentum Conservation 66

2.2.3. Description of Photoemission Process 68

2.2.4. Escape Depth of Photoelectrons 71

2.3. Spectral Function of ARPES 73

2.4. Analysis of ARPES 80

2.4.1. Energy & Momentum Distribution Curves 80

2.4.2. Matrix Element Effects 84

2.5. Analysis of CLPES 87

2.6. Experimental Details 93

2.6.1. Photon Source I: Synchrotron Radiation at PAL 93

2.6.2. Photon Source II: He-Discharge Lamp 96

2.6.3. Electron Analyzer 98

2.6.4. Sample Manipulator Design 102

2.6.5. Sample Preparation & Characterization 104

2.6.6. Other Technical Issues 107

Chapter 3. Nearly Massless Charge Carriers at Pb/Si Interface 110

3.1. Introduction & Strategy 111

3.2. Electronic Structure of the Pb/Si Interface 114

3.2.1. Overall Band Dispersions 114

3.2.2. Linear Energy Dispersions 117

3.3. Origin of Observed Bands 119

3.4. Mechanism for Linear Dispersion 122

3.5. General Relevance & Implications 125

3.6. Methods 128

3.6.1. Sample Preparation 128

3.6.2. ARPES Measurements 130

3.6.3. DFT Calculations 131

3.6.4. DFT Results Handling 131

3.6.5. Band Bending Calculations 133

3.6.6. k·p Modeling 133

Chapter 4. Growth of Pb Nanowires on Stepped Si(111) 136

4.1. Introduction 137

4.1.1. Overview 137

4.1.2. Backgrounds & Motives 137

4.2. Experimental Details 140

4.3. LEED Results & Phase Diagram 142

4.4. Coverage Estimation 146

4.5. Discussion on the LEED Results 147

4.6. Core-Level Photoemission Results 149

4.6.1. Pb 5d Spectra 149

4.6.2. Si 2p Spectra 151

4.7. Valence-Band Photoemission Results 157

4.8. Summary 159

Chapter 5. Strong Lateral Electron Coupling of Pb Nanowires 160

5.1. Introduction 161

5.1.1. Overview 161

5.1.2. Backgrounds & Motives 161

5.2. Experimental Details 163

5.3. Fabrication of Single-Domain Pb Nanowires 164

5.4. Microscopic Structure of Pb Nanowires 167

5.5. Electronic Structure of Pb Nanowires 171

5.6. Analysis & Interpretations 174

5.6.1. Tight Binding Analysis 174

5.6.2. Deduced Structure Model of Pb Nanowires 175

5.6.3. Step-Superlattice States 177

5.7. Stable 1D Conductance & Phase Transition 179

5.8. Summary 181

Chapter 6. Giant Kink in Electron Dispersion of Pb Nanowires 182

6.1. Introduction 183

6.1.1. Overview 183

6.1.2. Backgrounds & Motives 183

6.2. Experimental Details 188

6.3. Giant Kink in Electron Dispersion 189

6.4. Self-Energy Analysis 192

6.5. Origin of Giant Kinks 194

6.5.1. Non-Intrinsic Origin 194

6.5.2. Non-Fermi Liquids & Coupling to Collective Excitations 194

6.5.3. Electronic Kink Theory 195

6.6. Anisotropy of Giant Kink 197

6.7. Summary 201

Chapter 7. Conclusions 202

References 206

Abstract in Korean 222

List of Tables

Table 3.1: The effective mass values (m) obtained by the experiments and the calculation with k·p theory. Taken from Ref. 197. 122

Table 3.2: Velocity denotes the slope of dispersion at (or near) EF in m/s. Eo and Eg are the energy of the band edge and energy gap from a neighboring band, which are used for the k·p modeling. Mass denotes the effective mass (m) obtained by fitting experimental...(이미지참조) 134

Table 4.1: Major fitting parameters for the five components used to fit the Si 2p core-level spectra of the α×2 phase shown in Figure 4.8. The GW and SCLS's are consistent for different emission angles. The intensity of each component is given for three different... 155

List of Figures

Figure 1.1: Schematic illustrations for (top) ideal lattice structures in various low dimensions: 3D bulk of atoms, 2D sheet of atoms, 1D string of atoms and for (bottom) the corresponding Fermi-surface topologies of free electrons. 25

Figure 1.2: Development of the transistor size in integrated circuits versus time. Soon after the year 2030, the curve will reach the dimensions of a single atom. From Ref. 3 26

Figure 1.3: (a) Simple visualization of strong interactions between electrons in a 1D system. Electrons cannot escape from each other when moving along a line, which leads to the formation of collective excitations and the breakdown of the single electron picture. (b)... 28

Figure 1.4: Overview of CDWs in a 1D atom chain with a half electron fitting. The red balls are the atoms consisting of the 1D chain. The lines above the balls represent charge densities. The bottom part shows the respective band dispersions of 1D free electrons in the... 29

Figure 1.5: Response functions of free-electron gases in one-, two-, and three-dimensions. Taken from Ref. 17. 30

Figure 1.6: Cartoons showing the prototypical examples of low-dimensional materials. (a),(b) anisotropic bulk crystals: (a) Cuprates high-temperature superconductors, stacked 2D layers of the CuO₂ plane and the charge reservoir plane, where the chemical doping takes... 32

Figure 1.7: Schematic illustrations for various surface reconstructions: (a) Dimer-Adatom-Stacking fault (DAS) model for the Si(111)7×7 surface superstructure. (b) Low-dimensional structures of metal adsorbates (red balls) fabricated on the silicon surface (grey balls). 35

Figure 1.8: STM images for various low-dimensional structures realized on Si(111) with metal adsorbates. (center) bare Si(111)7×7. (a) array of Indium nanoclusters (0D), (b) array of Indium nanowires (1D), (c) lead overlayer (2D), (d) lead thin films and (e) lead... 37

Figure 1.9: (a) Microscopic images of a Si(557) surface with a periodicity of 5.73 nm, together with a side view of the unreconstructed unit cell. A single Si(111)7×7 unit is combined with a triple step that can be approximated by a Si(112) facet. The overview... 38

Figure 1.10: (a) Simplified 1D model of a periodic crystal potential terminating at an ideal surface. At the surface the model potential jumps abruptly to the vacuum level (solid line). The dashed line represents a more realistic picture, where the potential reaches the vacuum... 40

Figure 1.11: Fermi surfaces (top) and band dispersions (bottom) of (a) 2D Si(111)√3×√3-Ag at various levels of doping with extra Ag atoms and (b) of Si(553)-Au. In (a), the area of Fermi circles increases with the doping level (value above each panel in electrons/Si unit).... 41

Figure 1.12: Schematic illustrations for a few surface sensitive techniques: (a) STM (b) ARPES (c) surface conductivity measurements. 42

Figure 1.13: (a) Zigzag model for Si(111)4×1-In at RT. (b) Hexagon model for Si(111)8×2-In at low temperature. The dimerization and shear movements during the (4×1 ↔ 8×2 phase transition) are indicated by the arrows. From Ref. 96. STM topographs for Si(111)4×1-In... 44

Figure 1.14: (a) Fermi surface for Si(111)4×1-In at RT (b) underlying band dispersions at RT (above Tc, left) and at 45 K (below Tc, right). Taken from Refs. 62, 93.(이미지참조) 45

Figure 1.15: (a) Structural model for prototypical gold chain structures on stepped Si(111), Si(557)-Au. from Ref. 70. (b) It's STM image with the Au coverage 0.02 ML below optimum: there are a few patches of clean Si(111)7×7 left over forming long strips that are... 46

Figure 1.16: (a) Band dispersions for Si(557)-Au (left) and Si(553)-Au (right) near EF. Both exhibit a doublet of 1/2-filled bands, and Si(553)-Au has all extra fractionally-filled band. (b) Temperature dependence of the conductivity (circle) and resistance (cross) of the...(이미지참조) 47

Figure 1.17: STM topographs of Si(553)-Au at (a) 300 and (b) 45 K for an area of 10×10 nm² at 0.2 and 0.5 V biases (empty states), respectively. Taken from Ref. 68. 48

Figure 1.18: (a)-(c) Structure models for devil's stair case phases. two building block phases of (a) √7×√3 and (c) √3×√3. (b) An example of devil's staircase phases [the (1,1) phase], consisting of one √7×√3 and one √3×√3 unit cells. The phase notation was referred... 50

Figure 1.19: Evolution of the Fermi surface in dense Pb overlayers on Si(111). It has been suggested that the Fermi contours evolves systematically as Pb coverage changes. Taken from Ref. 78 51

Figure 1.20: Phase diagram for the dense Pb overlayers on Si(111). The thick arrows indicate the phases mainly focussed in this thesis varying the temperature (red) and coverage (blue), respectively. Reproduced from Ref. 120. 52

Figure 1.21: STM images of the Pb nanowires at (a) T = 100 K (22×16 nm²) and (b) T = 40 K (37×21 nm², The sample bias and the tunneling current are 0.5 V and 1 nA, respectively. Insets: Relief mode, emphasizing the weak modulation in (b) at 40 K that is absent in (a)... 53

Figure 1.22: (a) High-resolution STM image of the Pb nanowires taken at 78 K. (b) and (c) The structural model for Pb nanowires: (b) Pb monolayers sitting on the uniform step structures like a red carpet dressed on the stairs illustrated in (c). 54

Figure 1.23. (a) Conductance of the Pb nanowires measured as a function of temperature along the step-edge (σ∥, upper panel) aud the perpendicular direction (σ⊥, lower panel) (b) Conductance along the nanowires below Tc of 78 K versus 1/T. (c) Schematic drawing of...(이미지참조) 55

Figure 1.24: Description of two materials systems, the Pb overlayer on flat si(111) and the Pb nanowires on stepped Si(111), studied in this thesis. The red and white balls represent the Pb and Si atoms, respectively. 57

Figure 1.25: Chart to show the flow of issues in this thesis. They are topically divided into two parts on Pb overlayers (Part I.) and Pb nanowires (Part II.) 58

Figure 2.1: Schematic drawing of an early "photoemission" experiment. Light is sent on a film of an alkali metal (Na, K). The energy of the photoemitted electrons is measured by applying a retarding voltage. 61

Figure 2.2: Technological development in PES since the first observation of the Ag(111) surface state in photoemission spectra, showing vast improvements in instrumental resolution. For the data bottom, the peak width is dominated by intrinsic lifetime broadening, and... 63

Figure 2.3. Geometry of an ARPES experiment in which the emission direction of the photoelectron is specified by the polar (φ) and azimuthal (ψ) angles. 65

Figure 2.4: Schematic view of the photoemission process in the single particle picture. The electron energy distribution produced by incoming photons and measured as a function of the kinetic energy Ekin of the photoelectrons (right) is more conveniently expressed in terms...(이미지참조) 67

Figure 2.5: Illustration of the three-step model, with (1) optical excitation of an electron in the bulk, (2) transport of the photoelectron to the surface, and (3) escape of the photoelectron into vacuum free space. Taken from Ref. 80 70

Figure 2.6: Electron mean free path λ, measured for various metals, as a function of the kinetic energy. The solid line indicates the "universal curve" with a minimum of 2.5 Å in the kinetic energy range of 50-100 eV. Despite the universal character of the energy... 71

Figure 2.7: Illustration of the effects of interactions on the single-particle spectral function. On the left is the case of non-interacting electrons where the single-particle excitations are δ-function. On the right is the moderately interacting case where electron-electron interactions... 76

Figure 2.8: Simulation of A(k,ω) using a model self-energy. The solid and dashed lines show A(k,ω), and the coherent quasiparticle peak which was lineary expanded around Ek, respectively. The remaining spectral weight represents the incoherent part of the spectral...(이미지참조) 78

Figure 2.9: 2D spectral plot showing the intensity of photoelectrons as a function of the binding energy and the momentum. A cross section through the intensity at constant energy (ω = 0) as a function of momentum (an MDC), and a cross section through the intensity at... 81

Figure 2.10: Series of EDCs for the surface state of Be(0001) near EF taken at 15 K. The spectral functions calculated for the corresponding emission angles (solid lines) are compared. The dispersion shows an unusual lineshapes because of electron-phonon coupling....(이미지참조) 82

Figure 2.11: An illustration of the effects of electron-phonon coupling. (a) Electron-phonon coupling causes a distortion in the band dispersions near EF and generate the two pole structures. (b) Electron-hole pair excitations across the Fermi surface leading to Kohn... 83

Figure 2.12: Schematic representation of the polarization and photon energy effects in the photoemission process: (a) mirror plane emission, (b) sketch of the optical transition between atomic orbitals with different angular momenta (the wave functions of the harmonic... 85

Figure 2.13: (a) Initial/final state picture of CLPES for free atoms. In the first step, the core electron is removed while leaving the other electrons frozen in their original orbitals. In the second step, the other electrons are allowed to relax. This relaxation contributes... 89

Figure 2.14: Example of Doniach-Sunjic profiles with two different asymmetry parameters. 92

Figure 2.15: Schematic layout of the U7-beamline. U: undulator as a radiation source, J: jaws with copper plates, M1: condensing toroid mirror, S1: entrance slit, M2: plane mirror, G: plane grating, M3: refocusing cylindrical mirror, S2: exit slit, M4 and M5: variable radius... 94

Figure 2.16: Pictures taken for the U7-beamline (top) and the 8A2 endstation for the high-resolution ARPES (bottom). This station is equipped with a Scienta 2002 electron analyzer. 95

Figure 2.17: (a) Schematic drawing of VUV source head (VG-Scienta, Sweden). (b) Graph showing the relative intensities of multiple emissions from the He-discharge lamp (see text). The spectra were measured on the Al photodiode with a bias of -15 V. (c) Picture of VUV... 97

Figure 2.18: Pictures taken for the ARPES stations equipped with the high-performance Scienta electron analyzers and high-flux He-discharge sources: (top) Scienta 100 with an acceptance angle of ±4˚ and (bottom) the latest model of Scienta R4000 with a much wider... 99

Figure 2.19: (a) CAD drawing of SES R4000 electron analyzer (VG-Scienta, Sweden). (b) Schematic drawing of the internal structure of the analyzers. They can be categorized into three parts; the lens, hemispheres, and detector plates. (c) Enlarged image of detector part... 101

Figure 2.20: (a) CAD drawing of the low-temperature manipulator. The sample temperature can be cryogenically cooled down to 28 K. (b) Continuous mapping of the Fermi surfaces of Pb/Si(111) √7×√3 at various temperature, using the manipulator shown in (a), which... 103

Figure 2.21: Schematic illustration of the Knudsen-type cell evaporator (home-made). The head-shield part is not shown here. Taken from Ref. 188. 105

Figure 2.22: (a) LEED apparatus. Electrons thermally emitted from the filament are focussed onto the sample. Elastically scattered electrons are passed by the grids and accelerated onto the fluorescent collector grid. (b) Surface crystal truncation rods intersect the... 106

Figure 3.1: (a) Schematic illustration of the lattice and electronic structures of graphene. Taken from Ref. 190. (b) Cartoons showing the difference of band dispersions near EF between graphene and silicon.(이미지참조) 111

Figure 3.2: Simple calculations of k·p perturbation theory with the Kane model. Band dispersion becomes more linear as Eg → 0.(이미지참조) 112

Figure 3.3: Surface band dispersion of Ag/Si(111)√3×√3. The band dispersion of the Ag 5p surface states gets linear as the energy separation from the hybridized bands of Si 3p and Ag 5s states approaches to zero. Accordingly, the effective mass of the surface band (those... 113

Figure 3.4: Surface crystal structures for the well-established model of the Pb overlayer on Si(111) with a √7×√3 structure; (a) Top view and (b) side view. Pb atoms are densely packed within a single layer upon almost bulk-terminated Si(111) to form the... 114

Figure 3.5: (a) Reciprocal lattice structure of Pb /Si(111) with a √7×√3 structure. Grey and dashed lines represent √7×√3 and 1×1 symmetries, respectively. (b) and (c) ARPES data collected along (b) short and (c) long arrows in (a) (hv = 21.2 eV, T = 95 K), crossing... 115

Figure 3.6: Calculated shape of the band bending in n-type Si substrate (see the Methods section below for the details). Valence band maximum and conduction band minimum are plotted as a function of the distance perpendicular to the surface. 116

Figure 3.7: (a) ARPES intensity map of the R band. Data below the dashed lines are those symmetrized with respect to the Γs point in order to eliminate the strong neighboring feature S2. (b) Spectral peak positions of the R band extracted from MDCs shown in (c)... 118

Figure 3.8: (a) Constant energy contours at EF calculated from DFT based on the single-domain model and (b) after considering the overlap of triply-rotated domains. Contours from each domain [A, B, and C at the bottom of (b)] are indicated by different colors in...(이미지참조) 120

Figure 3.9: DFT bard dispersions along the arrow in Figure 3.8(b) for (a) domain A and (b) domains B and C, which are overlapped together in (c). The contributions from domains B and C are degenerated. The shaded area represents the projected bulk band structure. 121

Figure 3.10: Schematic illustration of the key mechanism for linear dispersion (extremely small-effective-mass value) in the inversion layers of semiconductors. VB (CB) denotes the valence (conduction) band. 123

Figure 3.11: (a)-(c) Schematics or surface state (SS) and LH band dispersions near Γ in Pb (a), Au (b), and Ag (c) overlayers on Si(111) with a common √3×3√ symmetry. (d)-(f) Corresponding ARPES dispersions of LH bands for (d) Pb, (e) Au, and (f) Ag systems taken... 124

Figure 3.12: (a) ARPES band dispersion of Au/Si(111)√3×√3 reported in Ref. 71. We noticed that the linear dispersion of Si-hole bands in ILs (near Γ as indicated by the red arrow) is clearly seen. (c) and (d) First principle calculations for the band dispersions of (c)... 126

Figure 3.13: (a) LEED image for triple domain Pb/Si(111)√7×√3 taken at 90 K with a primary electron energy of 81 eV. (b) Reciprocal lattice structure for the triple-domain Pb/Si(111)√7×√3 phase. The black dots denote the lattice points of Si(111)1×1, while... 129

Figure 3.14: Relationship of the transition temperature versus the lateral size of the domain. One set of data is taken with increasing sample temperature and the other with decreasing sample temperature. Taken from Ref. 124. 130

Figure 3.15: (a)-(c) Band dispersions calculated from DFT along the arrow in Figure 3.8 from domain A (a), from domains B and C (b), and the superimposed one of all triple domains (c). The shaded area represents the projected bulk band structure. All bands are... 132

Figure 4.1: (a) CoSi₂ nanowires is hundreds-nanometer scale. (b) Silicon nanowires self-assembled on the SiO₂/Si substrate in tens-nanometer scale. (c) Yt silicide nanowires self-assembled on Si(001) in sub-nanometer scale. From Refs. 113,222,223. 138

Figure 4.2: LEED patterns for different annealing temperatures after a deposition of 2 ML Pb on Si(557); (a) bare Si(557) before the deposition, (b) as Pb deposited without any annealing, and after an annealing at (c) 640, (d) 660, (e) 700, (f) 720, (g) 750, and (h) 850... 141

Figure 4.3: Detailed intensity profiles [(d), (e), and (f), respectively for (a), (b), and (c)] for the LEED patterns of (a) α×2, which gradually mixes up with [(b) and (c)] √3×10 as the annealing temperature increases. The profile is taken along the horizontal direction as... 143

Figure 4.4: Schematics of the surface morphology at different temperatures (phases) with different step-terrace configurations as deduced from the LEED results. The widths of terraces are given in the unit of the Si(111)1×1 lattice. 144

Figure 4.5: Schematics of structure models for the representative surface phases of Pb/Si(111). (a) The 1×1 phase at 1 ML (Ref. 235), (b) √3×√3 at 1.33 ML (Refs. 119,235), (c) √7×√3 at 1.0 ML (the trimer model, Refs. 124,235), and (d) √3×√3 at 1.2 ML (Refs.... 146

Figure 4.6: Pb 5d photoemission spectra for the series of phases of Si(557)-Pb shown in Figure 4.2. The spectra were taken at 70 K using the photon energy of 140 eV along a grazing emission angle of 60˚. All spectra are normalized by the peak intensity to show... 150

Figure 4.7: Si 2p photoemission spectra for the series of phases of Si(557)-Pb shown in Figure 4.2. The spectra were measured at 70 K using a photon energy of 140 eV along a grazing emission angle of 60˚ for the higher surface sensitivity. 152

Figure 4.8: The Si 2p photoemission spectra of the well-ordered α×2 phase taken at different emission angles with a photon energy of 140 eV. Open circles are the experimental data and the solid lines overlaid are fitting curves. The Lorentzian width of 0.045 eV is optimized,... 154

Figure 4.9: (a) The angle integrated valence-band spectra of Si(557)-Pb measured at 70 K with hv = 140 eV. (b) The spectrum of the α×2 phase (bottom one) near EF is closed up and compared to that of tantalum metal.(이미지참조) 158

Figure 5.1: Illustration of the recipe to fabricate Pb nanowires with an indirect heater. 163

Figure 5.2: LEED patterns of (a) the clean Si(557) surface, Pb-induced (b) streaky α×2, (c) and (d) spotty α × 2, and (e) β×2 phases. The incident electron energy was 80 eV. The unit cells are superimposed on (c)-(e). The phase diagram is summarized in (f). 165

Figure 5.3: Empty-state topographic STM images of the streaky (a) and the spotty (b) α×2 surfaces (70×70 nm²). The images (a) and (b) were taken at 87 and 78 K, respectively, with a sample bias (Vs) of 2.0 V, a tunneling current (It) of 0.30 nA and Vs = 0.5 V, It = 0.05 nA,...(이미지참조) 168

Figure 5.4: (a) The line profile along the "line α" in Figure 5.3(a). The α×2 phase is formed on the Si(223) facet which is cut from the Si(557) as shown in (b). 169

Figure 5.5: (a) STM topograph of the well-ordered Pb nanowires on Si(557) at 78 K with +0.5 V sample bias over an area of 40×22 nm², (b) enlarged image of the area within the dashed box in (a), and (c) height profile along the white line in (a). 170

Figure 5.6: (a) LEED pattern of the Pb nanowire phase at 70 K at 81 eV electron energy. (b) Front and (c) side views of the schematic model of the Pb nanowire structure; the red (blue) balls represent Pb (Si) atoms. The 42/3×2 unit cell is indicated by the white boxes.(이미지참조) 171

Figure 5.7: ARPES data of (a) Fermi surfaces and underlying band dispersions (b), (c) along and (d) perpendicular to the Pb nanowires at 70 K with photon energies of 21.2 eV and 140 eV (darker contrast for higher intensity). The schematics of the Fermi contours within... 172

Figure 5.8: The symmetrized map from the raw Fermi surface data of Figure 5.7(a) showing a wider k-space. The raw data taken over one quadrant (kx, ky) ≥ 0 of the k space are mirror symmetrized across x and y axes with subsequent translational operations. The diamond-...(이미지참조) 174

Figure 5.9: Simple tight-binding model considering only nearest-neighbor hopping and in-plane p orbitals. (a) Possible lattice models of a square and of a hexagon with the lattice constant of Si(111)1×1 (a0). (b) The result of tight-binding calculations with a square...(이미지참조) 176

Figure 5.10: Structure model of Pb nanowires considering the tight-binding analysis of the observed band structure with ARPES, step superstructures found in LEED, and real-space images taken by STM. The present system can be more properly described as Pb nanostripes... 177

Figure 5.11: Depending on the effective step potentials that electrons feel, the electron bands can be either step superlattice states (left) and lateral quantum well states (right). Reproduced from Ref. 248. 178

Figure 5.12: The splitting of large 2D Fermi contours into the multiple quasi-1D and 2D bands as small anti-crossing gaps open at the crossing points. This is the consequence of a unique feature of the present system that the Fermi wavevector of the original 2D bands... 179

Figure 5.13: (a) STM images and (b) LEED patterns above/below the phase transition temperature (Tc) reported previously and also recently. We found no temperature dependence at all both in microscopic and electronic structures. 180

Figure 6.1: Various degrees of freedoms in solids. Interactions between them are responsible for many exotic quantum phenomena such as charge/spin density waves, non-Fermi liquid behaviors, and the superconductivity. Reproduced from Refs. 50,257,258. 184

Figure 6.2: Schematic illustration to explain the kink structure in electron dispersion. The energy scale of the kink is directly relevant to the involved collective excitations, which couple to the electrons. From Ref. 162. 185

Figure 6.3: Giant kinks in electron dispersions reported previously on (a) transition-metal oxides (cuprates) from Ref. 260 and (b) graphene from Ref. 40. 186

Figure 6.4: Various models suggested to explain the giant kinks. (a) Coupling of electrons with collective excitations (here, electron-plasmons interaction), from Ref. 40. (b) Non-Fermi liquid behaviors, from Ref. 260. (c) Interaction between electrons within the Fermi-... 187

Figure 6.5: Illustration of fabrication of the patterned Pb nanowires (or nanoribbons) on the Si(557) substrate. 188

Figure 6.6: (a) STM topograph of the Pb/Si(557) at 78 K with +0.5 V sample bias over an area of 7.4×8.2 nm². The side view of the schematic structure model is at the bottom. The top (bottom) balls represent the Pb (Si) atoms, (b) The schematic Fermi surface reported... 189

Figure 6.7: (a) ARPES intensity map collected along the nanowires at 70 K with a photon energy of 80 eV. The measured k-space cut is indicated by arrows in Figure 6.6(b). Each band is tagged as in Figure 6.6(b). The parabolic lines are the dispersions of m2 and m3... 191

Figure 6.8: (a) Real part of self-energy Re∑(ω) obtained by taking the energy difference between the tight-binding and the measured dispersions. The line is the linear fit of Re∑(ω), whose slope corresponds to the coupling constant (λ). (b) Imaginary part of self-energy... 193

Figure 6.9: Self-energies for the couplings of electrons with collective excitations of (a) phonons and (b) plasmons. From Refs. 259, 280. 195

Figure 6.10: Schematic illustration to explain the electronic kink theory. ZFL denotes a renormalization factor, depending on the strength of electron correlations. The energy of the kink is determined by the point that the electron dispersion returns back to the bare-...(이미지참조) 196

Figure 6.11: Real and imaginary parts of the self-energy predicted in the electronic kink theory. From Ref. 269. 197

Figure 6.12: (a) A series of dispersions of the m4 band along the nanowires for different momentum cuts as shown in (b). Dots represent measured dispersions from MDC's while the lines are those calculated from the tight binding model. (b) Schematics of the Fermi.... 198

Figure 6.13: Schematic illustration for the changes in the electron band dispersions. Only the bands related to the diamond-shaped contour are depicted. The giant kink becomes noticeably enhanced as the measured k-cut approaches the saddle points of large 2D Fermi... 199

Figure 6.14: (a) A series of band dispersions of graphene for different momentum cuts shown in (b). (b) Fermi surface topology of electron-doped graphene showing the relationship between the singular points in the Fermi surface and electron-phonon coupling constants.... 200

초록보기

저차원 전자구조를 갖는 물질계(저차원 전자계)는 흥미로운 저차원 물리현상을 보여줄 뿐만 아니라 극소형 전자소자를 위한 잠재적 응용성 때문에 최근 20년간 지속적인 연구와 관심의 대상이 되어왔다. 특히 저차원 전자계는 통상적인 삼차원 물질들에는 존재하지 않는, 혹은 쉽게 관측할 수 없는, 여러 가지 물리현상을 관찰할 수 있다는 큰 장점을 갖는다. 기존에 많이 연구되어 오던 이방성이 큰 삼차원 물질계에 더하여, 최근에는 반도체 표면위에 자기조립되는 다양한 형태의 나노구조들이 - 예를 들면, 이차원 원자막과 일차원 원자선 등 - 새로운 저차원 전자계로서 주목받고 있다. 실제로 이러한 물질계는 뚜렷한 저차원 전자구조를 갖으며 스핀/전하 밀도파, 비페르미액체 현상 그리고 무질량 디랙(Dirac)입자와 같은 흥미로운 저차원 물리현상들을 보여주었다.

표면 나노구조들의 가장 큰 장점 중 하나는 이 물질계 특유의 "다양성"이라 할 수 있다. 나노구조를 형성하는 물질의 배합이나 화학량을 조절하여 서로 다른 구조와 주기를 갖는 다양한 이차원 상들을 체계적으로 유도해 낼 수 있다, 또한 비스듬한 기판을 이용할 경우에는 규칙적으로 정렬된 계단구조에 의해 비등방적인(일차원적인) 상을 유도할 수 있다. 그 대표적인 예로, 실리콘(111) 표면위에 자기 조립되는 원자 한 층 두께의 "이차원 납 원자막"을 들 수 있다. 이 물질계는 매우 복잡하고 독특한 상 그림을 갖는데, 그것은 소위 "악마의 계단"이라 불리는 수학적 이론모델로 설명된다. 다시 말해, 매우 적은 납 원자량에 민감하게 의존하여 무수히 많은 규칙적인 상들이 나타나며, 이들은 서로 조금씩 다른 주기와 형태의 띠구조를 갖는다. 뿐만 아니라, 납 원자막을 비스듬한 실리콘(111) [실리콘(557)] 기판위에 형성 시킬 경우, 수 나노미터 폭의 등 간격으로 잘 정렬된 "준 1차원 납 원자배선"을 구현할 수 있다. 실제로 납 원자배선에 관한 기존 연구는 극저온까지 안정적인 일차원적 금속 전도성을 보고하였다. 이와 같이 실리콘 기판위에 형성되는 납 원자선/원자막계에는 다양한 띠 혹은 계단구조를 갖는 여러 가지 상들이 존재하며, 이러한 특유의 구조적 "다양성"은 곧 그에 대응하는 다양한 전자구조를 체계적으로 연구할 수 있는 좋은 기회를 제공한다.

위와 같은 배경을 바탕으로, 본 학위논문에서는 고분해능 각도분해 광전자분광법을 활용하여 납 원자선/원자막 계의 전자구조를 연구하였다. 첫째로, 납 원자막에 관한 광전자 분광연구 결과, 관측된 표면 전자밴드 구조는 제1원리 밀도함수이론 계산 결과와 전반적으로 잘 부합하는 것으로 나타났다. 하지만, 납 원자막과 실리콘 기판의 계면 근처에 형성되는 실리콘 공간전하층에 분포하는 양공(hole)밴드는 독특한 선형의 밴드분산을 보였다. 선형 밴드분산은 통상적인 반도체들이 갖는 포물선형의 밴드분산과는 구분되며, 전하의 유효질량이 극단적으로 작은 "무질량 입자"에 가깝다는 것을 의미한다. 앞서 언급한 납 원자막의 다양한 전자구조를 체계적으로 비교/분석하여, 납원자막의 표면 전자밴드가 이웃한 실리콘 양공밴드의 분산을 선형화하는데 중요한 역할을 한다는 것을 유추해 낼 수 있었다. 관측한 밴드분산은 잘 알려진 k·p 섭동이론으로 잘 모사되며, 따라서 이 현상은 이웃한 두 전자밴드간의 반발 상호작용에 의한 것으로 설명할 수 있다. 본 결과는 표면 전자밴드와 기판의 전자밴드가 서로 이웃할 때 일어나는 반발 상호작용을 이용하여, 실리콘 계면에 근 무질량 입자를 유도해 낼 수 있음을 제시한다. 근 무질량 입자는 그 전하이동도가 매우 크기 때문에, 실리콘기반의 전자소자의 구동속도를 획기적으로 향상시키는 데 유용하게 활용될 수 있다. 뿐만 아니라 이러한 메커니즘은 특정 물질에 의존하지 않으므로, 여타 반도체 물질에도 응용할 수 있으며, 특히 III-V족 화합물 반도체에 고질적인 문제점에 해당하는 전자/양공이동도의 불균형 문제를 위한 유용한 해결책을 제시한다.

둘째로, 비스듬한 실리콘 기판위에 형성된 납 원자선의 경우, 주사터널링 현미경 그림 상에 매우 잘 정렬된 비등방적 구조로 나타난다. 하지만 이러한 일차원적인 구조에도 불구하고, 전자구조는 기본적으로 커다란 이차원 페르미면을 보이는 것을 발견하였다. 또한 이러한 이차원 페르미면들은 나노선의 수직방향으로 강한 일차원 변조효과를 보여 페르미면들이 서로 중첩되는 곳마다 작은 에너지 틈을 형성한다. 다시 말해 거대한 이차원 페르미면의 단순한 일차원 반복효과로 복잡한 전자구조를 모두 간단하게 이해할 수 있는 것이다. 이와 같은 전자구조 상의 이차원적인 그리고 준일차원적인 이중성은 기존에 보고되었던 납 원자선의 안정적인 일차원 금속 전도성을 잘 설명한다. 이차원 페르미면의 기원을 이해하기 위해 사각대칭성의 격자구조와 평면상의 p궤도를 가정하고 밀접결합모델(tight-binding model)계산을 수행하여 관측된 페르미면을 잘 재현해 낼 수 있었다. 따라서 납 원자선은 실제로는 수 나노미터 크기의 매우 좁은 테라스에 빽빽하게 밀집된 납 원자들로 구성되며, 국소적으로 강한 이차원 전자결합을 이룬다. 또한 원자선들끼리도 서로서로 전자적으로 강하게 결합하여 계단구조의 주기적인 퍼텐셜에너지에 의해 강하게 구속되지 않고 약하게 섭동받는 초격자 상태(superlattice states)로 이해할 수 있다. 더하여, 납 원자선의 밴드분산을 정밀하게 측정한 결과, 상대적으로 큰 에너지를 갖는 다체 상호작용의 전형적인 특징에 해당하는 "거대꼬임(giant kink)" 현상을 발견하였다. 이차원 납 원자막의 전자분산과 비교/대조를 통하여, 납 원자선의 줄어든 차원성과 변형된 격자구조가 다체 상호작용을 강화시킴을 유추해 낼 수 있었다. 관측된 밴드분산으로부터 자체에너지(self-energy) 분석을 시도한 결과, 거대꼬임 현상에 관한 여러 가지 이론모델 중 전자와 마그논(magnon) 그리고 전자와 플라스몬(plasmon) 상호작용 모델들은 실험 결과에 잘 맞지 않았다. 하지만 최근에 제시된 순수한 전자들간의 상호작용에 근거한 "전자적 꼬임이론(electronic kink theory)"은 발견된 거대꼬임의 에너지와 자체에너지 분석 결과를 잘 설명하는 것으로 나타났다. 본 연구 결과는 인위적으로 유도되는 나노차원의 원자배선에 대한 전자밴드구조 연구가 "전자의 다체 상호작용"과 같은 중요한 물리현상을 이해하는데 있어 새로운 접근법으로서 활용될 수 있다는 점을 제시한다.