The experiments on mirror DW manipulation and CDW AM characterization (Figs. 2 to 4 and figs. S4 and S5) were carried out in the MeV ultrafast electron diffraction (UED) setup in the Accelerator Structure Test Area facility at SLAC National Laboratory (34). Figure S1 shows a schematic of the setup. The 800-nm (1.55-eV), 80-fs pump pulse from a commercial Ti:sapphire regenerative amplifier (RA) laser (Vitara and Legend Elite HE, Coherent Inc.) was focused to a 150 μm × 150 μm (FWHM) area in the sample at an incidence angle of ~5°. The 3.1-MeV electron bunches with bunch length shorter than 150 fs were generated by radiofrequency photoinjectors. The electron beam was normally incident on the sample with a 90 μm × 90 μm (FWHM) spot size. No sample degradation occurred due to the illumination of the MeV electron source, as confirmed by the same diffraction pattern and the same CDW transition temperature TNC-C measured over several days. The laser and electron pulses were spatially overlapped on the sample, and their relative arrival time was adjusted by a linear translation stage. The diffraction pattern was imaged by a phosphor screen (P43) and recorded by an electron-multiplying charge-coupled device (CCD; Andor iXon Ultra 888). A circular through hole in the center of the phosphor screen allowed the passage of undiffracted electron beam to prevent camera saturation.

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