Pressure‐Induced Emission Luminogens Enable Optical Logic Gates Toward Lighting, Scintillators, and Anti‐Counterfeiting

The pressure‐induced emission luminogens (PIEgens) opened the door to highly emissive materials. However, the high‐pressure phase with excellent optoelectrical properties is difficult to stabilize at ambient conditions, seriously limiting the practical applications. Here, we first lighted up non‐emissive zero‐dimensional (0D) metal halide (C 25 H 22 P) 2 SnCl 6 via pressure engineering, ultimately yielding the bright emission. Note that the quenched (C 25 H 22 P) 2 SnCl 6 after pressure treatment of 20.0 GPa exhibited very bright blue–white emission. This irreversible photoluminescence (PL) transition was associated with irreversible amorphization by increasing the potential barrier of phase transition through the steric hindrance effect. The increased distortion of inorganic octahedra and the enhanced hydrogen bond interaction within the amorphous (C 25 H 22 P) 2 SnCl 6 after pressure treatment were responsible for the bright emission. Thus, pressure‐triggered PL turn‐on behavior can serve as a robust optical switchable logic gate from the initially dark state “0” to the bright state “1”. Furthermore, the pressure‐treated (C 25 H 22 P) 2 SnCl 6 exhibited an unexpected excitation‐dependent emission. The unique characteristic of “PIE” with different colors can be decoded the Morse code encrypted with the pressure‐treated (C 25 H 22 P) 2 SnCl 6 and different excitations. The quenched (C 25 H 22 P) 2 SnCl 6 ‐based phosphor‐converted light‐emitting diodes (pc‐LEDs), X‐ray dose rate detection and centimeter‐level patterns highlighted great potentials in lighting, display, scintillators, and anti‐counterfeiting.