Realizing Red Mechanoluminescence of ZnS: Mn2+ Through Ferromagnetic Coupling

Self‐recoverable mechanoluminescence (ML) is becoming a novel technology widely used in the fields of sensing, display, and artificial intelligence. The dominant ML material, ZnS: Mn2+, is reported to solely present a yellow emission color, which limits the applications of self‐recoverable ML materials to a large extent. Herein, an effective strategy to extend the ML emission range of ZnS: Mn2+ by the ferromagnetic coupling of Mn2+ ions are reported. Under the thermal carbon‐reduction atmosphere (TCRA), the emission ranges of ML, photoluminescence (PL), and persistent luminescence spectra of ZnS: Mn2+ phosphors are all successfully broadened from yellow to red. Furthermore, as for the PL and ML intensities of ZnS: Mn2+, they are intensified to 1.76 and 3.23 folds larger under the TCRA treatment than those in pure nitrogen, respectively. Various spectra and magnetic test results reveal that the red emission bands of ZnS: Mn2+ @TCRA phosphors originate from the ferromagnetic coupling of Mn2+ ions. This study is the first to realize strong red emission and tunable multicolor luminescence in the conventional ZnS‐based phosphors, which introduces opportunities for discovering the multiband emissions of Mn2+ ion in other compounds. Brightly multicolored ZnS: xMn2+ @TCRA elastic films have been fabricated to demonstrate their anti‐counterfeiting and security applications. Traditional ZnS: Mn2+ mechanoluminescent materials have been developed for realizing performance improvement and wavelength tunability. ZnS: Mn2+ sintered under a thermal carbon‐reducing atmosphere exhibits tunable blue‐to‐red, cyan‐to‐red, and yellow‐to‐red emissions under photo‐, thermal‐, and mechano‐stimulation, respectively, and has great potential for anti‐counterfeiting and security applications. This study provides opportunities to discover the multiband emission of Mn2+ ion in other compounds.