Khvichia Mariam, Chou Kai-Chun, Lee Sidney, Zeitz David C, Zou Shengli, Li Yan, Zhang Jin Z
Department of Chemistry and Biochemistry, University of California, Santa Cruz, California 95064, USA.
El Camino Community College, 16007 Crenshaw Blvd., Torrance, California 90506, USA.
J Chem Phys. 2024 Sep 21;161(11). doi: 10.1063/5.0222815.
We have synthesized L-cysteine and oleylamine stabilized CsPbBr3 perovskite quantum dots (PQDs) and coupled them with gold nanoparticles (AuNPs). The PQDs and AuNPs, as well as their hybrid nanostructures (HNS), were characterized using UV-visible (UV-vis) and photoluminescence (PL) spectroscopy. The UV-vis spectra show absorption bands of the HNS at 503 and 520 nm, attributed mainly to PQDs and AuNPs, respectively. The PQDs show a strong excitonic PL band peaked at 513 nm from PQDs. The HR-TEM results show the formation of hybrid structures between PQDs and AuNPs, which is also supported by the PL quenching of the PQDs by the coupled AuNPs. Ultrafast dynamics of the exciton and charge carriers in the HNS and pristine PQD were studied using femtosecond transient absorption. Multiexponential fitting of the dynamic data revealed the existence of shallow and deep trap states in pristine PQDs and ultrafast electron transfer from PQDs to AuNPs in the HNS. A kinetic model was proposed to account for the key dynamic processes involved and to extract the time for electron transfer from PQDs to AuNPs in the HNS, found to be ∼2 ps. Dynamic processes in pristine PQDs are largely unchanged by HNS formation with AuNPs.
我们合成了L-半胱氨酸和油胺稳定的CsPbBr₃钙钛矿量子点(PQDs),并将它们与金纳米颗粒(AuNPs)耦合。使用紫外可见(UV-vis)和光致发光(PL)光谱对PQDs、AuNPs及其混合纳米结构(HNS)进行了表征。UV-vis光谱显示HNS在503和520 nm处有吸收带,分别主要归因于PQDs和AuNPs。PQDs显示出一个在513 nm处达到峰值的强激子PL带。高分辨透射电子显微镜(HR-TEM)结果显示PQDs和AuNPs之间形成了混合结构,耦合的AuNPs对PQDs的PL猝灭也证实了这一点。使用飞秒瞬态吸收研究了HNS和原始PQD中激子和电荷载流子的超快动力学。对动力学数据的多指数拟合揭示了原始PQD中存在浅陷阱态和深陷阱态,以及HNS中从PQDs到AuNPs的超快电子转移。提出了一个动力学模型来解释所涉及的关键动力学过程,并提取HNS中从PQDs到AuNPs的电子转移时间,发现约为2 ps。原始PQD中的动力学过程在与AuNPs形成HNS后基本保持不变。