This PDF file includes:

• fig. S1. Powder XRD pattern of crushed MAPbBr₃ crystals.
• fig. S2. PL excitation spectrum and PL of a MAPbBr₃ single crystal measured at room temperature in ambient air.
• fig. S3. Photostability of MAPbBr₃ single crystal.
• fig. S4. PL spectra taken at different vacuum levels.
• fig. S5. PL spectra of crystals prepared by the AVC technique in vacuum and air.
• fig. S6. Steady-state and TRPL spectrum from a freshly cleaved crystal prepared by the ITC technique in vacuum and air.
• fig. S7. TRPL decay in vacuum from a crystal grown by ITC.
• fig. S8. PL intensity variation in different gases.
• fig. S9. Normalized PL spectra in different gases.
• fig. S10. PL intensity as a function of time in air under two-photon excitation (800 nm).
• fig. S11. Photocarrier distribution at t = 0 under single- and two-photon excitation conditions.
• fig. S12. TRPL spectrum from a crystal prepared by the ITC technique under lower power density of 400-nm excitation.
• References (43–45)

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Other Supplementary Material for this manuscript includes the following:

• movie S1 (.mp4 format). Perovskite crystal under excitation of a 400-nm wavelength laser from an atmosphere of air to vacuum and then to air.