Light propagation and nonlinear optical respnose in silver cluster-porphyrin nanostructures

该项目的目标是通过在选定的卟啉模板上自组装有序的银簇阵列，开发出新的优化设计的纳米结构，用于纳米光学器件，如传感器。我们将从理论上研究这些混合量子系统与局域电磁场相互作用的基本方面，并将制定控制相干光传播和局域化的策略。特别设计的具有最佳结构的卟啉低聚物以及扩展的一维和二维卟啉聚合物将用作模板来稳定尺寸选择银纳米团簇的有序阵列。我们将重点研究尺寸< 2nm的“类分子”簇，它们具有离散的电子态，局部吸收和发射以及相对较长的非辐射激发态寿命。基于项目第一阶段开发的方法，我们将使用时间相关密度泛函理论（TDDFT）结合计算电动力学来模拟这些系统中的非线性光学响应以及相干光的传播和定位。最优控制将用于控制光的传播，这是开发功能纳米光学器件的基础。该项目的最终目标是设计用于检测特定（生物）分子的新型纳米光学传感器。分析物分子结合位点的相干时空光定位将被利用，以提高检测选择性和灵敏度，远远超过目前的能力。

The goal of this project is to develop novel optimally designed nanostructures by selfassembling ordered arrays of silver clusters at selected porphyrin templates for the application in nanooptical devices such as sensors. We will theoretically investigate the fundamental aspects of the interaction of these hybrid quantum systems with localized electromagnetic fields and will develop strategies for the control of coherent light propagation and localization. Specifically designed porphyrin oligomers with optimal structures as well as extended one-dimensional and two-dimensional porphyrin polymers will be used as templates to stabilize ordered arrays of sizeselected silver nanoclusters. We will focus on “molecule-like” clusters with sizes <2 nm which exhibit discrete electronic states, localized absorption and emission and relatively long nonradiative excited state lifetimes. Based on the methodology developed in the first phase of the project, we will use time-dependent density functional theory (TDDFT) combined with computational electrodynamics in order to simulate the nonlinear optical response as well as the coherent light propagation and localization in these systems. The optimal control will be used to manipulate the light propagation, which is the basis for the development of functional nanooptical devices. The ultimate goal of the project is to design novel nanooptical sensors for the detection of specific (bio)molecules. The coherent spatio-temporal light localization at the binding site for the analyte molecule will be utilized in order to increase the detection selectivity and sensitivity far beyond the current cababilities.