1：Experimental Design and Method Selection:

The study utilized a high-power solid-state super-Gaussian continuous laser beam (Nd: YAG, wavelength = 1 μm) to irradiate the entire substrate through a quartz glass window with a spot size of 25 × 25 mm2. The deposition temperature was measured using an infrared pyrometer. The laser was operated in an open-loop mode, allowing the temperature to rise to a specific temperature at a certain laser power setting for immediate response, resulting in a heating rate of 500 K/s.

2：The deposition temperature was measured using an infrared pyrometer. The laser was operated in an open-loop mode, allowing the temperature to rise to a specific temperature at a certain laser power setting for immediate response, resulting in a heating rate of 500 K/s. Sample Selection and Data Sources:

2. Sample Selection and Data Sources: Graphene was grown on a 330 μm-thick 4H-SiC(0001) substrate (~10 × 5 mm2) with a Si-terminated polished face. Before placing the substrates into the chamber, they were cleaned following the Radio Corporation of America cleaning procedure.

3：List of Experimental Equipment and Materials:

High-power solid-state super-Gaussian continuous laser (Nd: YAG, wavelength = 1 μm), infrared pyrometer (Optris GmbH., Berlin, Germany), Raman spectroscopy (LabRAM HR Evolution; Horiba, Paris, France), atomic force microscopy (AFM, ICON2-SYS, Bruker, USA), cross-section TEM (JEOL JEM-2100 TITAN, Talos F200S, and Titan Cubed Themis G2 300), X-ray photoelectron spectroscopy (XPS, Multilab 2000, VG Inc.), ultraviolet photoelectron spectroscopy (UPS, Thermo ESCALAB 250XI), van der Pauw four-point probe Hall measurement system (HL5500 PC).

4：Experimental Procedures and Operational Workflow:

The SiC substrate was placed on a stage in a vacuum chamber with an Ar-gas flow and a pressure of 90 mbar. The laser was used to irradiate the entire substrate, and the sample was heated between 1550 °C and 1780 °C for 5 min. The number of layers and the quality of the obtained graphene were examined by Raman spectroscopy. The morphology was determined by AFM. Cross-section TEM images were used to determine the number of layers and stacking sequence of graphene. XPS and UPS were used to measure the binding energies and electronic structure, and the electrical properties were measured using a van der Pauw four-point probe Hall measurement system.

5：Data Analysis Methods:

The Raman spectra were analyzed to determine the quality and number of graphene layers. AFM and TEM images were analyzed to determine the morphology and stacking sequence of graphene. XPS and UPS data were analyzed to measure the binding energies and electronic structure. The electrical properties were analyzed using the van der Pauw four-point probe Hall measurement system.