Controlling Spin-Exchange Coupling and Energy Transfer at the Organic-Lanthanide Nanoparticle Interface

我们最近展示了通过将有机分子偶联到掺镧无机绝缘纳米颗粒来控制分子三重态动力学的可能性(han等人，《自然》2020)，为这些纳米系统在光电子学、光子频率转换、生物医学成像和光催化中的应用开辟了新的可能性。本项目将探索自旋一分子三重态与稀土离子之间的自旋交换耦合和能量转移的基本机制。获得机理洞察力的关键是精确控制分子和稀土纳米颗粒之间的界面。为了实现这一点，将在Bronstein Group(化学)中设计和合成分子配体，以控制这些界面上波函数的长度尺度和分子取向。这些配体的自组装将用FTIR、核磁共振和中子散射等技术来表征。系统的光物理和自旋性质将通过在Rao Group(物理)中的稳态和时间分辨光谱来研究。我们试图了解这些新发现的系统中波函数的基本性质，然后使用在设备应用中获得的见解，包括用于光子上下转换、成像和光催化的系统。

Our recent demonstration that it is possible to control molecular triplet dynamics by coupling organic molecules to lanthanide-doped inorganic insulating nanoparticles (Han et al, Nature 2020), opens new possibilities for the application of these nanosystems in applications in optoelectronics, photon frequency conversion, bio-medical imaging and photocatalysis. This project will explore the fundamental mechanisms of spin-exchange Coupling and energy transfer between the spin-one molecular triplet states and the lanthanide ions. Key to gaining mechanistic insights is the precise control of the interface between the molecules and the lanthanide nanoparticles. To achieve this molecular ligands will be designed and synthesized in the Bronstein Group (Chemistry), to control the length scales and molecular orientation of the wavefunctions at these interfaces. The self-assembly of these ligands will be characterised with techniques including FTIR, NMR and neutron scattering. The photophysical and spin properties of the system will then be studied via steady-state and time resolved spectroscopy in the Rao Group (Physics). We seek to understand the fundamental nature of wavefunctions in these newly discovered systems and then use the insights gained in device applications including systems for photon up and down conversion, imaging and photocatalysis.