Zhang Baowei, Goldoni Luca, Lambruschini Chiara, Moni Lisa, Imran Muhammad, Pianetti Andrea, Pinchetti Valerio, Brovelli Sergio, De Trizio Luca, Manna Liberato
Dipartimento di Chimica e Chimica Industriale, Università degli Studi di Genova, Via Dodecaneso 31, 16146 Genova, Italy.
Dipartimento di Scienza dei Materiali, Università degli Studi di Milano-Bicocca, via R. Cozzi 55, 20125 Milano, Italy.
Nano Lett. 2020 Dec 9;20(12):8847-8853. doi: 10.1021/acs.nanolett.0c03833. Epub 2020 Nov 17.
We employed oleylphosphonic acid (OLPA) for the synthesis of CsPbBr nanocrystals (NCs). Compared to phosphonic acids with linear alkyl chains, OLPA features a higher solubility in apolar solvents, allowing us to work at lower synthesis temperatures (100 °C), which in turn offer a good control over the NCs size. This can be reduced down to 5.0 nm, giving access to the strong quantum confinement regime. OLPA-based NCs form stable colloidal solutions at very low concentrations (∼1 nM), even when exposed to air. Such stability stems from the high solubility of OLPA in apolar solvents, which enables these molecules to reversibly bind/unbind to/from the NCs, preventing the NCs aggregation/precipitation. Small NCs feature efficient, blue-shifted emission and an ultraslow emission kinetics at cryogenic temperature, in striking difference to the fast decay of larger particles, suggesting that size-related exciton structure and/or trapping-detrapping dynamics determine the thermal equilibrium between coexisting radiative processes.
我们使用油基膦酸(OLPA)来合成CsPbBr纳米晶体(NCs)。与具有线性烷基链的膦酸相比,OLPA在非极性溶剂中具有更高的溶解度,这使我们能够在较低的合成温度(100°C)下进行反应,进而能够很好地控制NCs的尺寸。其尺寸可减小至5.0纳米,进入强量子限制区域。基于OLPA的NCs即使在极低浓度(约1 nM)下,甚至暴露于空气中时,也能形成稳定的胶体溶液。这种稳定性源于OLPA在非极性溶剂中的高溶解度,这使得这些分子能够与NCs可逆地结合/解离,防止NCs聚集/沉淀。小尺寸的NCs在低温下具有高效的、蓝移发射和极慢的发射动力学,这与较大颗粒的快速衰减形成显著差异,表明与尺寸相关的激子结构和/或俘获-脱俘获动力学决定了共存辐射过程之间的热平衡。