Solari Simon F, Poon Lok-Nga, Wörle Michael, Krumeich Frank, Li Yen-Ting, Chiu Yu-Cheng, Shih Chih-Jen
Institute for Chemical and Bioengineering, ETH Zürich, 8093 Zürich, Switzerland.
Laboratory of Inorganic Chemistry, ETH Zürich, 8093 Zürich, Switzerland.
J Am Chem Soc. 2022 Apr 6;144(13):5864-5870. doi: 10.1021/jacs.1c12294. Epub 2022 Mar 23.
Colloidal metal halide perovskite (MHP) nanocrystals (NCs) are an emerging class of fluorescent quantum dots (QDs) for next-generation optoelectronics. A great hurdle hindering practical applications, however, is their high lead content, where most attempts addressing the challenge in the literature compromised the material's optical performance or colloidal stability. Here, we present a postsynthetic approach that stabilizes the lead-reduced MHP NCs through high-entropy alloying. Upon doping the NCs with multiple elements in considerably high concentrations, the resulting high-entropy perovskite (HEP) NCs remain to possess excellent colloidal stability and narrowband emission, with even higher photoluminescence (PL) quantum yields, η, and shorter fluorescence lifetimes, τ. The formation of multiple phases containing mixed interstitial and doping phases is suggested by X-ray crystallography. Importantly, the crystalline phases with higher degrees of lattice expansion and lattice contraction can be stabilized upon high-entropy alloying. We show that the lead content can be approximately reduced by up to 55% upon high-entropy alloying. The findings reported here make one big step closer to the commercialization of perovskite NCs.
胶体金属卤化物钙钛矿(MHP)纳米晶体(NCs)是一类新兴的用于下一代光电子学的荧光量子点(QDs)。然而,阻碍其实际应用的一个巨大障碍是它们的高铅含量,在文献中,大多数应对这一挑战的尝试都损害了材料的光学性能或胶体稳定性。在此,我们提出一种后合成方法,通过高熵合金化来稳定铅含量降低的MHP NCs。在用多种元素以相当高的浓度对NCs进行掺杂后,所得的高熵钙钛矿(HEP)NCs仍具有优异的胶体稳定性和窄带发射,甚至具有更高的光致发光(PL)量子产率η和更短的荧光寿命τ。X射线晶体学表明形成了包含混合间隙相和掺杂相的多个相。重要的是,通过高熵合金化可以稳定具有更高晶格膨胀和晶格收缩程度的晶相。我们表明,通过高熵合金化,铅含量可大约降低多达55%。本文报道的这些发现使钙钛矿NCs向商业化迈进了一大步。