Controlling spin dynamics at room temperature in Lead-Halide Inspired Hybrid Semiconductors
Matthew Beard a
a National Renewable Energy Laboratory, 15013 Denver W Pkwy, Golden, CO 80401, United States
Materials for Sustainable Development Conference (MATSUS)
Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
#PeroQuant24 - Halide perovskites for quantum technologies
Barcelona, Spain, 2024 March 4th - 8th
Organizers: Simon Boehme, Sascha Feldmann and Maksym Kovalenko
Invited Speaker, Matthew Beard, presentation 289
DOI: https://doi.org/10.29363/nanoge.matsus.2024.289
Publication date: 18th December 2023

In this presentation I will discuss our studies of controlling spin populations in metal-halide organic/inorganic hybrid systems. Lower dimensional perovskites are of particular interest since the lower degree of symmetry of the metal-halide connected octahedra and the large spin-orbit coupling can potentially lift the spin degeneracy. To achieve their full application potential, an understanding of spin-relaxation in these systems are needed. Here, we report an intriguing spin-selective excitation of excitons in a series of 2D lead iodide perovskite (n = 1) single crystals by using time- and polarization-resolved transient reflection spectroscopy as well as transient circular dichroism. Exciton spin relaxation times are studied at room temperature for a range of 2D lead iodide perovskite systems and correlated to the exciton binding energy and degree of distortion in the metal halide framework. We also studied the spin-dynamics using THz emission spectroscopy and report on the circular photogalvanic and spin photogalvanic effect. Finally we are also investigating a novel class of chiral hybrid semiconductors based upon layered metal-halide perovskite 2D Ruddlesden-Popper type structures. These systems exhibit chiral induced spin selectivity (CISS) whereby only one spin sense can transport across the chiral layer and the other spin sense is blocked for one handedness of the chiral perovskite layer. We show that chiral perovskite layers are able to achieve > 80% spin-current polarization. I will discuss studies of spin-injection into a chiral-layer.

I aknowledge support for this work as part of the Center for Hybrid Organic Inorganic Semiconductors for Energy (CHOISE) funded by the Office of Science within the US Department of Energy.  

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