Department of Biophysics, Faculty of Biotechnology, University of Wrocław, F. Joliot-Curie 14a str, 50-383 Wrocław, Poland.
Department of Biophysics, Faculty of Physics, Astronomy and Informatics, Nicolaus Copernicus University, Grudziądzka 5 str., 87-100 Toruń, Poland.
Phys Chem Chem Phys. 2021 Nov 3;23(42):24505-24517. doi: 10.1039/d1cp03347f.
In this study, we investigated an experimental and Monte-Carlo computational characterization of self-assembled antennae built using CdTe colloidal quantum dots (QDs). These clusters provide efficient excitation of phycocyanine (PC) or phycobilisomes (PBSs). PBSs are light-harvesting complexes (LHCs) of cyanobacteria, made of several PC units, organized in disks and rods. Each PC contains three separate cofactors. Therefore, we analyzed variations in multi-donor and multi-acceptor systems. The self-assembled QD clusters were formed mostly by electrostatic interactions, possibly due to the introduction of a positive charge on an originally negatively charged nanoparticle surface. Our results suggest that PC may accept energy from multiple nanoparticles localized at a distance significantly longer than the Förster radius. The excitation transfers between particular nanoparticles with possible delocalization. The maximal energy transfer efficiency was obtained for the PC/PBS : QD ratio from 1 to 20 depending on the QD size. This cannot be fully explained using computational simulations; hence, we discussed the hypothesis and explained the observations. Our self-assembled systems may be considered for possible applications in artificial light-harvesting systems because absorption spectra of QDs are different from the absorption characteristics of PC/PBS. In addition, huge clusters of QDs may effectively increase the optical cross-section of so-created nanohybrids.
在这项研究中，我们研究了使用 CdTe 胶体量子点 (QD) 自组装天线的实验和蒙特卡罗计算特性。这些簇为藻蓝蛋白 (PC) 或藻胆体 (PBS) 的有效激发提供了条件。PBS 是蓝藻的光捕获复合物 (LHC)，由几个 PC 单元组成，组织在圆盘和棒状结构中。每个 PC 包含三个独立的辅因子。因此，我们分析了多供体和多受体系统的变化。自组装的 QD 簇主要通过静电相互作用形成，这可能是由于原本带负电荷的纳米颗粒表面引入了正电荷。我们的结果表明，PC 可能会从多个位于明显长于Förster 半径的距离的局部化纳米粒子中接受能量。能量在特定的纳米粒子之间转移，可能会发生离域化。对于 PC/PBS:QD 比值为 1 到 20 的比例，获得了最大的能量转移效率，这取决于 QD 的尺寸。这不能用计算模拟完全解释，因此，我们讨论了假设并解释了观察结果。我们的自组装系统可以考虑用于人工光捕获系统，因为 QD 的吸收光谱与 PC/PBS 的吸收特性不同。此外，QD 的巨大簇可能会有效地增加如此创建的纳米杂化物的光学横截面。
