Executive Summary : | Understanding light-matter interaction is crucial in physical, chemical, and material sciences, owing to a variety of applications, for instance, in optically tuned information technology devices, in lasers and lighting, and solar-energy harvesting, as well as in storage and sensors. Developing materials with new functionalities and combinations thereof is vital in designing molecular species with technologically relevant properties. Coordination chemistry offers a versatile platform for preparing multifunctional molecular solids with tunable physical properties that may be in synergy. In addition, the size of these materials containing two different components can be reduced to the nanoscale for useful applications. The project proposed herein seeks to advance our understanding of the stimuli-responsive structure-function relationship in multifunctional molecule-based materials and nanostructures, followed by their device application. Firstly, we aim to design new multifunctional molecular materials based on the combination of Fe(II) spin-crossover (SCO) complexes with substituted 1,2,4-triazole ligands and Ln(III) (Ln = Eu, Tb) coordination complexes with variable diketonate ligands. We intend to synthesize and characterize a molecular system where the usually particular wavelength to trigger a volume change transition in an SCO material can be broadened by incorporating a Ln(III) component near the iron ion. This goal would function as a light-controlled molecular actuator under a broad range of wavelengths. Secondly, this proposal aims to prepare coordination nano-objects possessing two physical properties in synergy: molecular SCO and luminescent lanthanides, to design novel ultrasensitive and adjustable nanothermometers for application in biology, for example. However, we focus here on the design and assessment of the physical behavior of the nano-objects, not on the biological application part. Finally, we aim to integrate such coordination networks, including nanostructures, into photoresponsive metal-insulator-metal (MIM) capacitor design and fabricate hybrid inorganic-organic photoresponsive Field Effect Transistors (FETs) for superior performance. In particular, we propose (i) the fabrication of MIM based capacitor by exploiting photoresponsive bistability states on the dielectric properties of the materials, (ii) a fundamental understanding of MIM device fabrication will be further exploited in the design and fabrication of photoresponsive bistable FETs. In the FET geometry, combined SCO-Ln molecular materials and nanostructures will be used as gate dielectric material with different device geometry, including floating gate configuration. Therefore, this proposal establishes a novel synthetic and experimental approach for the incorporation of multifunctionality into molecular materials and nanostructures fundamentally and from a device fabrication standpoint. |