Publication date: 3rd June 2020
The structural, optical, and magnetic properties of the vacancy-ordered quadruple perovskites Cs4CdBi2Cl12 and Cs4MnBi2Cl12 and their solid solution have been investigated. Both compounds are found to crystallize with R3 m space group symmetry that arises from ordering of Bi3+, Mn2+/Cd2+, and cation vacancies into layers that run perpendicular to the <111> direction of the cubic perovskite structure. Magnetic measurements reveal that Cs4MnBi2Cl12 is paramagnetic down to 2 K with a Weiss constant of −2.88(3) K and an effective moment of 5.840(1) μB. This compound exhibits weak orange-red luminescence, which involves Bi3+ ions absorbing near UV photons followed by energy transfer to Mn2+ ions and finally radiative decay that is attributed to a spin-forbidden 4T1(G) ® 6A1(S) d–d transition. The emission peak is centered near 605 nm and has a full-width-half-maximum of ~90 nm and a photoluminescent quantum yield (PLQY) of ~ 4%. The isostructural Cs4CdBi2Cl12 is neither magnetic nor does it show detectable photoluminescence at room temperature. Replacing Mn2+ with Cd2+ to form Cs4Cd1−xMnxBi2Cl12 leads to a zero-dimensional electronic structure that inhibits energy migration to defect sites where non-radiative decay can occur, increasing the room temperature PLQY to 57% in the x = 0.27 sample. Cs4Cd1−xMnxBi2Cl12 phosphors are easily synthesized from solution, free of rare-earth ions, and possess emission spectra that compare favorably to narrow-band red emitting phosphors based on Eu2+ ions.
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