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See supplementary material at for supplementary Figure S1 which shows infrared transmittance spectra from Bi2Te3at temperatures of 287 K and 390 K. In Figure S2, we indicate the time constant of the decrease and recovery in the mid-infrared probe reflectance spectroscopy. Figure S3 shows the infrared-to-visible reflectivity spectrum at room temperature. Figure S4 shows that the time evolution of the electron diffraction intensity from the planes corresponds to spot 1–6 and that the time evolution from the planes corresponds to spots 7 and 8. Figure S5 shows the time-resolved change in the diffuse scattering background. Figure S6 shows the time-resolved electron intensity from the diffraction plane. Figure S7 shows atomic displacements derived from the time-resolved electron diffraction. Figure S8 shows the Raman spectrum and the coherent phonon vibrations determined from the conventional near-IR pump-probe experiment. Tables S1–S7 present the atomic coordinates obtained from the time-resolved electron diffraction.[Supplementary Material]
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The atomic and electronic dynamics in the topological insulator (TI) BiTe under strong photoexcitation were characterized with time-resolved electron diffraction and time-resolved mid-infrared spectroscopy. Three-dimensional TIs characterized as bulk insulators with an electronic conduction surface band have shown a variety of exotic responses in terms of electronic transport when observed under conditions of applied pressure, magnetic field, or circularly polarized light. However, the atomic motions and their correlation between electronic systems in TIs under strong photoexcitation have not been explored. The artificial and transient modification of the electronic structures in TIs via photoinduced atomic motions represents a novel mechanism for providing a comparable level of bandgap control. The results of time-domain crystallography indicate that photoexcitation induces two-step atomic motions: first bismuth and then tellurium center-symmetric displacements. These atomic motions in BiTe trigger 10% bulk bandgap narrowing, which is consistent with the time-resolved mid-infrared spectroscopy results.


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