Figure 1.1. Cross-section of the crust and mantle showing the main location of diamond formation in... 30

Figure 1.2. Lattice structure of a diamond unit cell, ao is the cubic lattice parameter. The image origin... 32

Figure 1.3. Lattice structure of (a) Diamond and (b) Graphite. The images are from Zigya.com with... 32

Figure 1.4. (a) Dark current for a CVD-diamond film during first hnear heatmg and cooling in dry air.... 34

Figure 1.5. Experimental data on both pure Ila diamond and BDDs. The image is from Figure 5 in Ref.25 35

Figure 1.6. Examples of minerals at each level on the Mohs Hardness Scale. The image is from... 36

Figure 1.7. Cyclic voltammograms before and after for diamond (a and b), HOPG (c and d), and glassy... 37

Figure 1.8. Optical microscopy (OM) images of (a) diamond, (b) HOPG and (c) Glassy carbon after... 38

Figure 1.9. The schematic illustration of a NV center (a), a SiV center (b) and a BV center (c) in... 39

Figure 1.10. Timeline of selected events in the history of the laboratory grown diamond. The image is... 40

Figure 1.11. Scheme of HPHT process. (a) A HPHT belt-type chamber. The figure shows a few... 41

Figure 1.12. Diamond product synthesized by HPHT shown different colors. (a) This collection of... 42

Figure 1.13. The scheme shows the process of PECVD. The image is from Figure 2 in Ref.72 43

Figure 1.14. (a)The scheme shows the setup of polycrystalline diamond growth by HFCVD. (b)... 45

Figure 1.15. (a) SEM images of the surface (up) and the cross section (down) of a diamond film grown... 46

Figure 1.16. The scheme shows the process of DND method. The image is from Daicel Corporation... 47

Figure 1.17. (a) The scheme shows the configuration of device (Galinstan was used as interconnects... 49

Figure 1.18. Direct ink writing of printed parts with programmable LM microstructure. (a) Optical... 50

Figure 1.19. (a) Schematic illustration of the process of the low-temperature graphene growth using a... 52

Figure 1.20. Hydrogen production with a Ni-Bi molten catalyst in the bubble column they built. The... 53

Figure 1.21. A summary of thermodynamic properties of eligible metal candidates for participation in... 54

Figure 1.22. Schematic illustration the experiment setup and the process of CO₂ dissociation in liquid... 55

Figure 2.1. (a) Carbon phase diagram as a function of pressure and temperature. (b) The scheme shows... 57

Figure 2.2. Photographs of the (a) home-built cold-wall system for diamond growth, and the... 59

Figure 2.3. Scheme showing the different regions (positions) at which temperatures were measured by... 63

Figure 2.4. 'Quenching' experiments 64

Figure 2.5. Raman spectroscopy of graphite crucible (GC, 'cavity bottom surface') and EDM-3 Poco... 66

Figure 2.6. The experiment without liquid metal. (a) The low magnification SEM image and (b) the... 67

Figure 2.7. SEM images of the center region of 5 different solidified liquid metal pieces after growths... 68

Figure 2.8. SEM images showing the diamond found at the center regions of the bottom of the solidified... 69

Figure 2.9. SEM images showing the growth at the center regions of the solidified liquid metal piece... 69

Figure 2.10. SEM images showing the growth at the center regions of the solidified liquid metal piece... 70

Figure 2.11. SEM images showing the growth at the center regions of the solidified liquid metal piece... 71

Figure 2.12. SEM images showing the growths found at the center regions of the solidified liquid metal... 72

Figure 2.13. SEM images and Raman spectra of the growths with no H₂ present. (a, b) The growth with... 73

Figure 2.14. SEM images and Raman spectra of the growths with different ratios of CH₄ / H₂. (a, b)... 74

Figure 2.15. SEM images and EDS analysis of the growth using 20/100 CH₄/H₂. (a) Low magnification... 75

Figure 2.16. (a) Scheme of the experimental setup: A graphite crucible with cavity is the Joule-heated... 76

Figure 2.17. (a) A photo showing the as-grown diamond on the solidified liquid metal surface after a... 77

Figure 2.18. SEM image of a diamond film after growth for 300 min 77

Figure 2.19. AFM measurements of the thickness of diamond films that were transferred to Quantifoil... 78

Figure 2.20. SEM images of the diamonds grown at the center of the bottom surface of the metal alloy.... 79

Figure 2.21. SEM images of diamond crystals after growth for (d) 15 min, (e) 30 min, (f) 60 min, and... 79

Figure 2.22. SEM images showing as-grown diamonds 'buried' (partially) in solidified liquid metal... 80

Figure 2.23. SEM image of the as-grown diamond for a growth time of 60 min 80

Figure 2.24. SEM images of the as-grown diamond film for a growth time of 150 min. (a) Low... 81

Figure 2.25. Tilted SEM images (tilt angle 50°) of the as-grown diamond regions for 3 different growth... 81

Figure 2.26. ToF-SIMS spectra of the back side of the as-transferred diamond film (a) C. (b) Ga. (c) Si.... 82

Figure 2.27. XPS spectra of (a) Ga 2P₃/₂ and (b) Si 2P for the back side of as-transferred diamond film 83

Figure 2.28. (a) An optical image of the as-transferred diamond film on a Quantifoil holey amorphous... 83

Figure 2.29. Optical image of an as-transferred diamond film on a 300 nm SiO₂/Si wafer 84

Figure 2.30. Plan-view TEM images of a diamond film from a growth of 150 mm as-transferred on a... 85

Figure 2.31. (a) Plan view TEM image of a diamond film (150 min growth) after transfer onto Cu TEM... 85

Figure 2.32. Cls XPS spectrum measured from a transferred diamond film on a 300 nm SiO₂/Si wafer.... 85

Figure 2.33. ToF-SIMS depth-profiling (Intensity as function of the depth) obtained on as-grown... 86

Figure 2.34. Raman analysis (obtained with 266 nm laser) of as-grown diamond film after transferring... 86

Figure 2.35. (a) ZPL peak of the as-grown diamonds compared to the as-grown graphite, excited by a... 87

Figure 2.36. Characterization of ¹³C-labeled as-grown diamond, (a) Scheme of the three configurations... 88

Figure 2.37. The growth result with ¹³CH₄ for 150 min at 1175 ℃ by inserting one piece of HOPG... 89

Figure 2.38. A growth run with a PBN (pyrolytic boron nitride) plate placed at the bottom of graphite... 90

Figure 2.39. (a-b) SEM images of the bottom surface of the EDM-3 Poco Graphite sheet (the side that... 91

Figure 2.40. SEM images of (a) ¹³C- D150-GC, (b) ¹³C-150D-EDM, and (c) ¹³C-D150-SEDM 91

Figure 2.41. UV Raman analysis of the ¹³C-D150-EDM and ¹³C-D150-GC. (a) The Raman map of ID/IG...[이미지참조] 92

Figure 2.42. Raman map of ¹³D intensity of the same region as Fig.2c for sample ¹³C-D150-EDM 92

Figure 2.43. Raman spectra of the as-grown diamonds obtained with normal methane 93

Figure 2.44. ToF-SIMS surface spectra of the D-labeled as-grown diamond film (solidified liquid... 94

Figure 2.45. SEM image and UV Raman analysis of the D-labeled as-grown diamond film, (a) SEM... 95

Figure 2.46. ToF-SIMS surface spectra of the solidified liquid metal for the CH₄/D₂ (5/100) run at 50,... 95

Figure 2.47. (a-b) Computed radial distribution function (RDF) of liquid Ga at (a) 375 and (b) 1300 K... 97

Figure 2.48. (a-b) Optimized structure of (a) CH₄(ads) and (b) CH₃(ads) + H(ads) on Ga slab surface... 97

Figure 2.49. Data calculated from HSC Chemistry. HSC Chemistry is a software package including... 98

Figure 2.50. (a) Formation energy per atom in 120 Ga liquid metal (orange column) and in the Ga-Fe-... 103

Figure 2.51. Relative total energies of Si-C-C, C-Si-C, Fe-C-C, and F-C-C-Si and their structures. There... 103

Figure 2.52. Projected DOS of the indicated clusters. (a-b) PDOS for a single atom in Ga-Ni-Fe solvent:... 105

Figure 2.53. Projected DOS and is structure when carbon interacts with many surrounding Ni and Fe... 106

Figure 2.54. (a) The structure of the solute is shown by excluding the 120 Ga in the slab structure of... 106

Figure 2.55. (a) PDOS of the structure shown in Fig. S53a. (b) PDOS of the structure shown in Fig.... 107

Figure 2.56. (a) Structure before and after 5 ps MD in liquid Ga of C₁₀ structure with all hydrogen... 108

Figure 2.57. (a-c) PDOS of (a) The C₁₀ cluster described in the text, (b) the C₁₀ chain that forms, and... 108

Figure 2.58. (a) TEM image of the as-grown diamond (D) film and the graphite (G) film beneath the... 109

Figure 2.59. Raman depth profiling for the as-grown diamond regions. (The same sample, but not the... 110

Figure 2.60. HR-TEM image obtained from the region in Figure 2.58a showing the interface between... 110

Figure 2.61. TEM data of cross-section sample (D150) prepared by SEM-FIB. (a) Large-area cross-... 112

Figure 2.62. TEM data of cross-section sample (D30) prepared by SEM-FIB. (a) Large-area cross-... 113

Figure 2.63. (a) HR-TEM image of the Ml region of D30 (inset: FFT pattern). It shows that the M1... 114

Figure 2.64. (a) Cross section TEM image showing the region contained D1 and the metal beneath D1... 114

Figure 2.65. TEM-EDS analysis of carbon concentration in M1 and M2 of sample D30. (a) Cross-... 115

Figure 2.66. ToF-SIMS depth-profiling of carbon (¹³C⁻) concentrations obtained on two different... 117

Figure 2.67. Scheme showing the growth of diamond at the bottom surface of the liquid metal 118

Figure 2.68. TEM-EDS line profiling showing silicon concentration with depth. (a-c) TEM images of... 119

Figure 2.69. ToF SIMS depth-profiling of silicon concentrations (ion counts as function of the depth... 120

Figure 2.70. Binary phase diagram of Sn, In, Pb and Bi with Ni and Fe, respectively. (a) Sn/Ni. (b)... 123

Figure 2.71. The experiment of Sn replacing Ga. The SEM image (a) and Raman spectrum (b) show... 124

Figure 2.72. The experiment of In replacing Ga. SEM image (a) and Raman spectrum (b) show the... 124

Figure 2.73. The growth result for the liquid metal composed of 0.25 at% Si, 14.67 at% Ni, 7.33 at%... 125

Figure 2.74. (a) A photograph (note green colored region), (b) an SEM image, and (c) Raman spectra:... 126

Figure 2.75. Growth runs with quartz or sapphire substrates placed between graphite crucible and liquid... 126

Figure 3.1. SEM images of NGD regions grown on SCDS-100 with different concentrations of silicon... 131

Figure 3.2. SEM images of NGD regions on SCDS-100 samples that were each heated at 900 ℃ for... 132

Figure 3.3. SEM images of NGD regions obtained by annealing SCDS-100 for 12h at each of the... 133

Figure 3.4. SEM images of NGD regions obtained by annealing SCDS-100 in a liquid Ga (Si) mixture... 134

Figure 3.5. SEM images of new growth attempts on substrates other than diamond. Annealing at 900... 134

Figure 3.6. SEM images of different NGDs on SCDS-110. (a and b) Obtained by annealing SCDS-110... 135

Figure 3.7. Homoepitaxial diamonds grow on SCDS-100. (a) Schematic of the quartz tube furnace with... 136

Figure 3.8. SEM image and EDS spectrum of new diamond growth (NGD) obtained on the SCDS-100... 137

Figure 3.9. Silicon carbide by-product, (a) SEM image of a region containing the silicon carbide by-... 137

Figure 3.10. Homoepitaxial new growth pyramid diamond on SCDS. (a) Cross-section TEM image of... 138

Figure 3.11. Homoepitaxy at the interface between a grown pyramid and the substrate. (a) Cross-... 139

Figure 3.12. TEM characteristics of 3C-SiC particles on the diamond substrate. (a) Cross-section image... 140

Figure 3.13. 3C-SiC crystals on apex of pyramid diamonds. (a) SEM image of NGD grown on SCDS-... 141

Figure 3.14. GI-SAXS experimental set-up and GI-SAXS patterns. (a) Illustration of the GI-SAXS... 142

Figure 3.15. GI-SAXS analysis of NGD samples on SCDS-100 with azimuth. (a) Azimuthal angle... 143

Figure 3.16. Incident angle dependent GI-SAXS patterns measured at azimuthal angle Ω ＝ 0°.... 144

Figure 3.17. WAXD pattern of new diamond growth (NGD-2) sample obtained on the SCDS-100. (a)... 145

Figure 3.18. GI-SAXS patterns measured at azimuthal angles Ω ＝ 0° and 45°. (a and b) GI-SAXS... 146

Figure 3.19. (a) Diagram of tilting sample 35.0°. (b) SEM image of pyramid without tilt. (c) Sample... 146

Figure 3.20. SEM tilting studies. (a) Diagram of tilting of an NGD-SCSD-100 sample (Annealing at... 147

Figure 3.21. Raman spectra of as-received SCDS and ¹³C-labeled NGD on the SCDS. (a) Raman... 148

Figure 3.22. Sequential growth. SEM images of NGD growth after different times. The sample was... 149

Figure 3.23. Kinetics of pyramid diamonds grown on SCDS-100. (a-c) Typical SEM images of NGD... 150

Figure 4.1. (a) The photo shows liquid gallium and GalP (G-O) (3.6. wt% G-O) on glass slides. (b) The... 155

Figure 4.2. Photographs of Pure Ga and GalP (G-O) on various metal surfaces. (a) (top) Pure liquid... 156

Figure 4.3. Photographs detailing the preparation of GalP (G-O) using plastic labware, (a) Pure liquid... 157

Figure 4.4. GalP (G-O) is highly processable and versatile; it can be readily reshaped to a five-pointed... 158

Figure 4.5. Customization of GalP (G-O) by molding. (a) A rod (or fiber), a plate (or film) and bulk... 159

Figure 4.6. Differential scanning calorimetry (DSC) of GalP. (a) GalP (G-O), melting point: 31.9. ℃.... 159

Figure 4.7. (a) The photo showing that GalP (G-O) can be either soft or stiff depending on the... 159

Figure 4.8. Photographs showing the effect of freezing on both GalP (G-O) and pure Ga. (a) GalP (G-... 160

Figure 4.9. (a) SEM image of GalP (G-O); pink dotted lines indicate some pores generated by the... 161

Figure 4.10. Chemical characterization of GalP (G-O). (a) Raman spectrum, (b) XRD pattern, and (c)... 161

Figure 4.11. Optical microscope and SEM images of GalP (G-O). (a) Optical microscope image of the... 161

Figure 4.12. (a) Viscosity of GalP (G-O) (with different G-O mass loading) under different shear rates.... 162

Figure 4.13. Mechanical strength of GalP block, plate and rod. (a) Compressive test of a bulk GalP (G-... 163

Figure 4.14. Photos showing how the particle size affects the incorporation. (a) silicon carbide, (b)... 164

Figure 4.15. The mixability of synthetic diamond powders with varying particle sizes (Diamond... 165

Figure 4.16. SEM images showing how the small particles are wrapped by Ga oxide and form a separate... 166

Figure 4.17. XPS spectra of a Ga oxidelayer on the surface of a liquid Ga droplet. (a) (left) Photograph... 167

Figure 4.18. Scanning transmission electron microscope (STEM) images of GalP (D, ≈11 μm) with... 168

Figure 4.19. Lower magnification STEM images GalP (D, ≈11 μm) with overlays of STEM-EDS... 169

Figure 4.20. (a) Illustration of the formation mechanism of GalP; the particle size and Ga oxide layer... 170

Figure 4.21. Illustration of the preparation of GalP (G-O). (a) Schematic of the mechanism of the... 170

Figure 4.22. Effect of filler volume on the formation of GalP. Illustration showing as the filler volume... 171

Figure 4.23. Eutectic putty prepared by mixing G-O with EGaln, EGaSn and Galinstan. The high... 172

Figure 4.24. (a) The photo shows liquid gallium on the commercial silicone putty. (b) The photo shows... 172

Figure 4.25. Mechanical strength of eutectic gallium putties. (a, b) Tensile and compressive stress-... 173

Figure 4.26. Fabrication of the porous Ga / rG-O foam. SEM image of a porous Ga/rG-O foam. Inset:... 174

Figure 4.27. Photos showing the volume changes of GalP (G-O) putty plate and cylinder while being... 174

Figure 4.28. Thermogravimetric analysis coupled with mass spectrometry (TGA-MS) of GalP (G-O).... 175

Figure 4.29. Volume expansion of GalP (G-O) with different G-O mass loadings as a function of... 176

Figure 4.30. Optical photos showing a piece of GalP (G-O) was heated at different temperatures and a... 176

Figure 4.31. Left photo shows the exterior and interior of a Ga/rG-O foam; right photo shows that the... 177

Figure 4.32. (a) Photos showing a piece of commercial A4 paper with GalP (rG-O) coating. The photos... 177

Figure 4.33. SEM image of the cross section of an rG-O/GalP (rG-O) film. Inset: Photo showing the... 178

Figure 4.34. (a)Tensile strain-stress curves of a rG-O and rG-O/GalP (rG-O) film. (b) The GalP (rG-O)... 178

Figure 4.35. SEM images, thermal conductivities and diffusivities of GalP (D). (a, b) SEM images of... 179

Figure 4.36. Thermal diffusivity and conductivity of GalP (rG-O) and GalP (D) parallel and... 180

Figure 4.37. Test system configuration for demonstrating the perpendicular heat transfer capability of... 180