Photoexcitation has been utilized to control quantum matter and to uncover metastable phases far from equilibrium. Among demonstrations to date, the most common is the photoinduced transition from correlated insulators to metallic states; however, the reverse process without initial orders has not been observed. Here, we show ultrafast metal-to-insulator transition in gate-doped ${\mathrm{WS}}_2/{\mathrm{WSe}}_2$ and ${\mathrm{WSe}}_2/{\mathrm{WSe}}_2$ moiré devices using photothermionic hole injection from graphite gates. The resulting correlated insulators are metastable, with lifetimes exceeding microseconds. These findings establish an effective mechanism for the ultrafast control of correlated electronic phases in van der Waals (vdW) heterostructures.

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• Photoinduced effect
• Quantum phase transitions