White-Light Emission and Structural Distortion in New Corrugated Two-Dimensional Lead Bromide Perovskites

Hybrid inorganic-organic perovskites are developing rapidly as high performance semiconductors. Recently, two-dimensional (2D) perovskites were found to have white-light, broadband emission in the visible range that was attributed mainly to the role of self-trapped excitons (STEs). Here, we describe three new 2D lead bromide perovskites incorporating a series of bifunctional ammonium dications as templates which also emit white light: (1) α-(DMEN)PbBr₄ (DMEN = 2-(dimethylamino)ethylamine), which adopts a unique corrugated layered structure in space group Pbca with unit cell a = 18.901(4) Å, b = 11.782(2) Å, and c = 23.680(5) Å; (2) (DMAPA)PbBr₄ (DMAPA = 3-(dimethylamino)-1-propylamine), which crystallizes in P2₁/c with a = 10.717(2) Å, b = 11.735(2) Å, c = 12.127(2) Å, and β = 111.53(3)°; and (3) (DMABA)PbBr₄ (DMABA = 4-dimethylaminobutylamine), which adopts Aba2 with a = 41.685(8) Å, b = 23.962(5) Å, and c = 12.000(2) Å. Photoluminescence (PL) studies show a correlation between the distortion of the "PbBr₆" octahedron in the 2D layer and the broadening of PL emission, with the most distorted structure having the broadest emission (183 nm full width at half-maximum) and longest lifetime (τ_avg = 1.39 ns). The most distorted member α-(DMEN)PbBr₄ exhibits white-light emission with a color rendering index (CRI) of 73 which is similar to a fluorescent light source and correlated color temperature (CCT) of 7863 K, producing "cold" white light.