Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO <sub>3</sub> Thin Films

The search for thin film electro-optic materials that can retain superior performance under cryogenic conditions has become critical for quantum computing. Barium titanate thin films show large linear electro-optic coefficients in the tetragonal phase at room temperature, which is severely degraded down to ≈200 pm V<sup>-1</sup> in the rhombohedral phase at cryogenic temperatures. There is immense interest in manipulating these phase transformations and retaining superior electro-optic properties down to liquid helium temperature. Utilizing the thermodynamic theory of optical properties, a large low-temperature electro-optic response is designed by engineering the energetic competition between different ferroelectric phases, leading to a low-symmetry monoclinic phase with a massive electro-optic response. The existence of this phase is demonstrated in a strain-tuned BaTiO<sub>3</sub> thin film that exhibits a linear electro-optic coefficient of 2516 ± 100 pm V<sup>-1</sup> at 5 K, which is an order of magnitude higher than the best reported performance thus far. Importantly, the electro-optic coefficient increases by 100 × during cooling, unlike the conventional films, where it degrades. Further, at the lowest temperature, significant higher order electro-optic responses also emerge. These results represent a new framework for designing materials with property enhancements by stabilizing highly tunable metastable phases with strain.

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Publication Details

Journal
Advanced Materials
Published
2025-10-11
DOI
https://doi.org/10.1002/adma.202507564
Primary Topic
Ferroelectric and Piezoelectric Materials
Type
article
Field-Weighted Citation Impact
0.00

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article

Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO 3 Thin Films

Suchismita Sarker, Sankalpa Hazra, Albert Suceava, Venkatraman Gopalan et al.
Advanced Materials
Ferroelectric and Piezoelectric Materials
article

Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO 3 Thin Films

Suchismita Sarker, Sankalpa Hazra, Albert Suceava, Venkatraman Gopalan, Saugata Sarker, Aiden Ross, Vladimir A. Stoica, Himirkanti Sarkar, Darrell G. Schlom, Yingxin Zhu, Dylan Sotir, Long‐Qing Chen, Yang Yang, Zhiyu Zhang, Lei Ding, Brynn Brower, Ian Reed Philippi
article en

Abstract

The search for thin film electro-optic materials that can retain superior performance under cryogenic conditions has become critical for quantum computing. Barium titanate thin films show large linear electro-optic coefficients in the tetragonal phase at room temperature, which is severely degraded down to ≈200 pm V<sup>-1</sup> in the rhombohedral phase at cryogenic temperatures. There is immense interest in manipulating these phase transformations and retaining superior electro-optic properties down to liquid helium temperature. Utilizing the thermodynamic theory of optical properties, a large low-temperature electro-optic response is designed by engineering the energetic competition between different ferroelectric phases, leading to a low-symmetry monoclinic phase with a massive electro-optic response. The existence of this phase is demonstrated in a strain-tuned BaTiO<sub>3</sub> thin film that exhibits a linear electro-optic coefficient of 2516 ± 100 pm V<sup>-1</sup> at 5 K, which is an order of magnitude higher than the best reported performance thus far. Importantly, the electro-optic coefficient increases by 100 × during cooling, unlike the conventional films, where it degrades. Further, at the lowest temperature, significant higher order electro-optic responses also emerge. These results represent a new framework for designing materials with property enhancements by stabilizing highly tunable metastable phases with strain.

Advanced MaterialsVol. 38(3)
Pennsylvania State University (US), Cornell University (US), Interface (United States) (US), Leibniz Institute for Crystal Growth (DE)
National Science Foundation, U.S. Department of Energy, University of Pennsylvania, Pennsylvania State University, Office of Science, Materials Research Science and Engineering Center, Harvard University, Division of Materials Research, Basic Energy Sciences, Brookhaven National Laboratory, Energy Frontier Research Centers
Openalex Percentile: Top 78%
Ferroelectric and Piezoelectric Materials
DOIOpen Access PDFOpenAlex
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