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金掺杂对原子精确的银配位纳米团簇双光子吸收和发光的影响。

Gold-Doping Effect on Two-Photon Absorption and Luminescence of Atomically Precise Silver Ligated Nanoclusters.

作者信息

Pniakowska Anna, Kumaranchira Ramankutty Krishnadas, Obstarczyk Patryk, Perić Bakulić Martina, Sanader Maršić Željka, Bonačić-Koutecký Vlasta, Bürgi Thomas, Olesiak-Bańska Joanna

机构信息

Institute of Advanced Materials, Wroclaw University of Science and Technology, Wybrzeże Wyspiańskiego 27, 50-370, Wroclaw, Poland.

Département de Chimie Physique, Université de Genève, 30 Quai Ernest-Ansermet, 1211, Geneva 4, Switzerland.

出版信息

Angew Chem Int Ed Engl. 2022 Oct 24;61(43):e202209645. doi: 10.1002/anie.202209645. Epub 2022 Sep 14.

Abstract

Noble metal nanoclusters allow for the atomically-precise control of their composition. However, to create nanoclusters with pre-defined optical properties, comprehensive description of their structure-property relation is required. Here, we report the gold atom doping impact on one-photon and two-photon absorption (TPA) and luminescence properties of ligated silver nanoclusters via combined experimental studies and time-dependent density functional theory simulations (TD-DFT). We synthesized a series of Ag Au (DMBT) nanoclusters where x=0, 1 and 5-10. For Ag Au (DMBT) we demonstrate that the presence of the central Au dopant strongly influences linear and non-linear optical properties, increasing photoluminescence quantum yield and two-photon brightness, with respect to undoped silver nanoclusters. With improved TPA and luminescence, atomically-precise AuAg alloys presented in our work can serve as robust luminescent probes e.g. for bioimaging in the second biological window.

摘要

贵金属纳米团簇能够对其组成进行原子级精确控制。然而,要制备具有预定义光学性质的纳米团簇,需要全面描述其结构与性质的关系。在此,我们通过结合实验研究和含时密度泛函理论模拟(TD-DFT),报告了金原子掺杂对连接的银纳米团簇的单光子和双光子吸收(TPA)以及发光性质的影响。我们合成了一系列AgₓAu₁₋ₓ(DMBT)纳米团簇,其中x = 0、1以及5 - 10。对于AgₓAu₁₋ₓ(DMBT),我们证明相对于未掺杂的银纳米团簇,中心金掺杂剂的存在强烈影响线性和非线性光学性质,提高了光致发光量子产率和双光子亮度。凭借改进的TPA和发光性能,我们工作中呈现的原子级精确的AuAg合金可作为强大的发光探针,例如用于第二生物窗口的生物成像。

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