(PECASE) MULTI-DIMENSIONAL VIBRATIONAL-ELECTRONIC SPECTROSCOPY
Abstract
We describe the application of novel time-resolved spectroscopic methods in order to understand and exploit coupled energy transfer processes in hybrid nanostructured materials. We aim to apply single-shot ultrabroadband multi-dimensional coherent spectroscopy to directly observe the dynamics that accompany electronic-to-vibrational energy transfer (EVET) processes at organic/inorganic interfaces. Specifically, we aim to study energy repartitioning at the sub-nano scale through coherent and incoherent energy exchange from highlying excitonic states of quantum dots (QDs) to the vibrational modes of the organic ligands. Study of these basic EVET processes using the proposed techniques will provide quantitative measurements of energy repartitioning at chemical and structural discontinuities, and will elucidate the interactions that control dynamics. The goals of this project may be summarized as: Goal 1: to measure and predictively model the rates of EVET processes in solution-phase and thin-films of semiconductor QDs. Goal 2: to use our mechanistic understanding of EVET processes to design QD architectures and surface chemistries to control the redistribution of energy across a heterogeneous (organicinorganic) interface. Achieving these goals will allow a deeper understanding of the basic physics describing EVET, which has important applications - for instance, the collision of nanoscale materials with highly energetic molecules. The resilience of these systems relies in large part on their ability to redistribute charge and energy dynamically at nanoscopic structural and chemical discontinuities. Specifically, we will utilize powerful light sources across wide spans of the electromagnetic spectrum, combined with high-order nonlinear spectroscopy with detection modalities that will dramatically increase sensitivity and resolution over the state-of-the-art (SOA).
Document Details
- Document Type
- DoD Grant Award
- Publication Date
- Aug 12, 2021
- Source ID
- FA95502010175
Entities
People
- Elad Harel
Organizations
- Air Force Office of Scientific Research
- Michigan State University
- United States Air Force