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

preprint
submitted on 09.01.2020 and posted on 10.01.2020 by Stephen Londo, Somnath Biswas, Jakub Husek, Igor V. Pinchuk, Michael J. Newburger, Alexandra Boyadzhiev, Amanda H. Trout, David W. McComb, Roland Kawakami, L. Robert Baker
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.

Funding

Probing Ion Solvation and Charge Transfer at Electrochemical Interfaces Using Nonlinear Soft X Ray Spectroscopy

Basic Energy Sciences

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NSF MRSEC DMR-1420451

History

Email Address of Submitting Author

baker.2364@osu.edu

Institution

The Ohio State University

Country

United States

ORCID For Submitting Author

0000-0001-6740-864X

Declaration of Conflict of Interest

None

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