Sørensen Lasse K, Gerasimov Valeriy S, Karpov Sergey V, Ågren Hans
Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, Odense M DK-5230, Denmark.
University Library, University of Southern Denmark, DK-5230 Odense M, Denmark.
Phys Chem Chem Phys. 2024 Sep 25;26(37):24209-24245. doi: 10.1039/d4cp00778f.
Plasmonics serves as a most outstanding feature of nanoparticle technology and is nowadays used in numerous applications within imaging, sensing and energy harvesting, like plasmonically enhanced solar cells, nanoparticle bioimaging, plasmon-controlled fluorescence for molecular tracking in living cells, plasmon-controlled electronic molecular devices and surface enhanced Raman spectroscopy for single molecular detection. Although plasmonics has been utilized since ancient times, the understanding of its basic interactions has not been fully achieved even under the emergence of modern nanoscience. In particular, it has been difficult to address the "ultra-fine" 1-10 nm regime, important for applications especially in bioimaging and biomedical areas, where neither classical nor quantum based theoretical methods apply. Recently, new approaches have been put forward to bridge this size gap based on semi-empirical discrete interaction models where each atom makes a difference. A primary aim of this perspective article is to review some of the most salient features of these models, and in particular focus on a recent extension - the extended discrete interaction model (Ex-DIM), where the geometric and environmental features are extended - and highlight a set of benchmark studies using this model concerning size, shape, material, temperature dependence and other characteristics of ultra-fine plasmonic nanoparticles. We also analyze new possibilities offered by the model for designing ultra-fine plasmonic particles for applications in the areas of bioimaging, biosensing, photothermal therapy, infrared light harvesting and photodetection. We foresee that future modelling activities will be closely connected to collaborative experimental work including synthesis, device fabrication and measurements with feedback and validation in a systematic fashion. With this strategy we can expect that modelling of ultra-fine plasmonics particles can be integrated in the development of novel plasmonic systems with unprecedented performance and applicability.
等离激元学是纳米粒子技术最为突出的特性，如今已应用于成像、传感和能量收集等众多领域，如等离激元增强太阳能电池、纳米粒子生物成像、用于活细胞分子追踪的等离激元控制荧光、等离激元控制电子分子器件以及用于单分子检测的表面增强拉曼光谱。尽管等离激元学自古以来就已被利用，但即使在现代纳米科学出现之后，对其基本相互作用的理解仍未完全实现。特别是，对于“超精细”的1 - 10纳米范围，尤其是在生物成像和生物医学领域的应用而言至关重要，但经典理论方法和基于量子的理论方法在此都不适用，因此一直难以解决这一问题。最近，基于半经验离散相互作用模型提出了新方法来弥合这一尺寸差距，在该模型中每个原子都起着重要作用。这篇观点文章的主要目的是回顾这些模型的一些最显著特征，尤其关注最近的扩展——扩展离散相互作用模型（Ex - DIM），其中几何和环境特征得到了扩展——并重点介绍一组使用该模型进行的关于超精细等离激元纳米粒子的尺寸、形状、材料、温度依赖性及其他特性的基准研究。我们还分析了该模型为设计用于生物成像、生物传感、光热疗法、红外光收集和光检测等领域的超精细等离激元粒子所提供的新可能性。我们预见，未来的建模活动将与合作实验工作紧密相连，包括以系统的方式进行合成、器件制造以及带有反馈和验证的测量。通过这种策略，我们可以预期超精细等离激元粒子的建模能够融入具有前所未有的性能和适用性的新型等离激元系统的开发中。
