Ultrafast Spin Crossover in a Room-Temperature Ferrimagnet: Element-Specific Spin Dynamics in Photoexcited Cobalt Ferrite

10 January 2020, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

Transition metal complexes capable of photo - induced spin crossover have been widely investigated because of their potential to enable ultrafast optical control of information processing. However, any real application of photo-switchable molecules requires that spin crossover be paired with additional functionality such as long-range magnetic order. Important advances combining these functions are notably reported for a number of bimetallic Prussian Blue analogues; however, to date PBA-based magnetic photo-switches can only operate be-low 150 K due to loss of magnetic order. In contrast, cobalt ferrite is a ferrimagnetic semiconductor with a Curie temperature of 790 K and extremely favorable magnetic properties by comparison to state-of-the-art PBAs. The mixed valence electronic structure of cobalt ferrite is reminiscent of cobalt-iron PBA, which is a well-known photo-switch. To investigate the potential for photo-switching in this material, we employ transient XUV spectroscopy to probe charge and spin dynamics with element-speci fic resolution on the femtosecond time scale. Results show that 400 nm light excites a metal-to-metal charge transfer transition, which drives the crossover of high-spin Co2+ to low-spin Co3+ with a time constant of 405 ± 29 fs and an internal quantum efficiency of unity. This result establishes the existence of efficient photo-switching in a new class of robust ferrimagnetic spinel ferrites.

Keywords

Spin crossover
XUV
M-edge XANES
Cobalt ferrite
Spinel ferrite

Supplementary materials

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