Deterministic optical control of room temperature multiferroicity in BiFeO3 thin films

Abstract

Controlling ferroic orders (ferroelectricity, ferromagnetism and ferroelasticity) by optical methods is a significant challenge due to the large mismatch in energy scales between the order parameter coupling strengths and the incident photons. Here, we demonstrate an approach to manipulate multiple ferroic orders in an epitaxial mixed-phase BiFeO3 thin film at ambient temperature via laser illumination. Phase-field simulations indicate that a light-driven flexoelectric effect allows the targeted formation of ordered domains. We also achieved precise sequential laser writing and erasure of different domain patterns, which demonstrates a deterministic optical control of multiferroicity at room temperature. As ferroic orders directly influence susceptibility and conductivity in complex materials, our results not only shed light on the optical control of multiple functionalities, but also suggest possible developments for optoelectronics and related applications.

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Fig. 1: Optical modulation of the highly strained BFO thin film.
Fig. 2: The ferroelectric configuration of a highly-strained BFO thin film after light illumination.
Fig. 3: Raman scattering study on the illuminated area.
Fig. 4: Phase-field simulations and flexoelectric effect under illumination.
Fig. 5: Optical control of room-temperature multiferroicity in BFO and creating designer domain architectures via laser-spot motion.
Fig. 6: Deterministic optical control of piezoelectric property in mixed-phase BFO.

Data availability

The data supporting the findings of this study are available within the article and its supplementary files and available from the authors upon reasonable request.

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Acknowledgements

This work is supported by the Ministry of Science and Technology (MOST) in Taiwan under grant nos. MOST 107-2636-M-006-003 (Young Scholar Fellowship Program), 105-2112-M-006-001-MY3, 106-2119-M-009-011-MY3, 106-2628-E-009-001-MY2 and 107-2627-E-006-001. Y.-H.C. acknowledges financial support from Academia Sinica, Taiwan (iMATE-107-11) and the Center for Emergent Functional Matter Science at National Chiao Tung University. R.T.H. and Y.C. acknowledge the Texas Advanced Computing Center (TACC) at The University of Texas at Austin for providing HPC resources that have contributed to the research results reported within this paper (http://www.tacc.utexas.edu). C.-Y.K., C.-T.C., C.-F.C. and L.H.T. acknowledge support from the Max-POSTECH/Hsinchu Center for Complex Phase Materials, and thank H.-M. Tsai, H.-W. Fu and C.-Y. Hua for their skilful technical assistance. V.N. acknowledges support from the Australian Research Council Discovery Project. This research used resources of the Advanced Light Source, which is a DOE Office of Science User Facility under contract no. DE-AC02-05CH11231.

Author information

J.-C.Y., Y.-L.H. and Y.-H.C. processed the sample growth. Y.-D.L. and Y.-Y.C. conducted the laser illumination, Raman spectroscopy and scanning probe microscopy, and analysed the data. R.T.H. and Y.C. conducted the phase-field simulation. Y.-C.W. and H.-J.L. processed the X-ray reciprocal mapping and resolved the phase transformation at elevated temperature. R.V.C. acquired and analysed the PEEM results. C.-Y.K., C.-T.C., A.T., C.-F.C. and L.H.T. measured and analysed X-ray absorption spectroscopy and XLD, and conducted the cluster calculation. V.N. analysed the PFM data and provided guidance on related experiments. Y.-C.C. and J.-C.Y. conceived the idea, led the project, analysed data and co-wrote the paper. All the authors contributed to the manuscript.

Correspondence to Yi-Chun Chen or Jan-Chi Yang.

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Supplementary Figs. 1–12 and Supplementary references 1–15.

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