Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO3 Thin Films

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

doi:10.1002/adma.202507564

Title: Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO₃ Thin Films

Journal Article · Sat Oct 11 00:00:00 UTC 2025 · Advanced Materials

DOI: https://doi.org/10.1002/adma.202507564 · OSTI ID:3012961

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^[1]; Philippi, Ian Reed ^[2];

^[3]; Brower, Brynn ^[1]; Ding, Lei ^[1]; Zhu, Yingxin ^[1];

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Pennsylvania State Univ., University Park, PA (United States)
Pennsylvania State University University Park PA 16802 USA
Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States); Leibniz Inst. for Crystal Growth (IKZ), Berlin (Germany)

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⁻¹ 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 BaTiO₃ thin film that exhibits a linear electro-optic coefficient of 2516 ± 100 pm V⁻¹ 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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Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012375; SC0012704; SC0020145; SC0021118

OSTI ID:: 3012961

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 3 Vol. 38; ISSN 1521-4095; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (59)

Tuning the Electro‐Optic Properties of BaTiO₃ Epitaxial Thin Films via Buffer Layer‐Controlled Polarization Rotation Paths Yu, Han; Guo, Ning; Deng, Chenguang Advanced Functional Materials, Vol. 34, Issue 30 https://doi.org/10.1002/adfm.202315579	journal	March 2024
Electro‐Optic Modulation in Hybrid Metal Halide Perovskites Gao, Yuan; Walters, Grant; Qin, Ying Advanced Materials, Vol. 31, Issue 16 https://doi.org/10.1002/adma.201808336	journal	February 2019
Linear Electro‐Optic Modulation in Highly Polarizable Organic Perovskites Sun, Meng‐Jia; Zheng, Chao; Gao, Yuan Advanced Materials, Vol. 33, Issue 4 https://doi.org/10.1002/adma.202006368	journal	December 2020
Colossal Strain Tuning of Ferroelectric Transitions in KNbO₃ Thin Films Hazra, Sankalpa; Schwaigert, Tobias; Ross, Aiden Advanced Materials, Vol. 36, Issue 52 https://doi.org/10.1002/adma.202408664	journal	November 2024
Enhanced Electro‐Optic Coefficients in Single‐Crystalline BaTiO₃ Thin Films Enabled by Domain Alignment Wen, Yiyang; Cao, Yilin; Chen, Haisheng Advanced Optical Materials, Vol. 12, Issue 15 https://doi.org/10.1002/adom.202303058	journal	April 2024
Coherent Conversion Between Microwave and Optical Photons—An Overview of Physical Implementations Lambert, Nicholas J.; Rueda, Alfredo; Sedlmeir, Florian Advanced Quantum Technologies, Vol. 3, Issue 1 https://doi.org/10.1002/qute.201900077	journal	January 2020
Measurement of the electro-optic coefficients: description and comparison of the experimental techniques Aillerie, M.; Théofanous, N.; Fontana, M. D. Applied Physics B: Lasers and Optics, Vol. 70, Issue 3 https://doi.org/10.1007/s003400050053	journal	March 2000
Effect of substrate constraint on the stability and evolution of ferroelectric domain structures in thin films Li, Y. L.; Hu, S. Y.; Liu, Z. K. Acta Materialia, Vol. 50, Issue 2 https://doi.org/10.1016/S1359-6454(01)00360-3	journal	January 2002
Properties of rare-earth scandate single crystals (Re=Nd−Dy) Uecker, R.; Velickov, B.; Klimm, D. Journal of Crystal Growth, Vol. 310, Issue 10 https://doi.org/10.1016/j.jcrysgro.2008.01.019	journal	May 2008
Light scattering models for describing the transmittance of transparent and translucent alumina and zirconia ceramics Pabst, Willi; Hříbalová, Soňa Journal of the European Ceramic Society, Vol. 41, Issue 3 https://doi.org/10.1016/j.jeurceramsoc.2020.10.025	journal	March 2021
Analysis of the Pockels effect in ferroelectric barium titanate thin films on Si(0 0 1) Kormondy, Kristy J.; Abel, Stefan; Fallegger, Florian Microelectronic Engineering, Vol. 147 https://doi.org/10.1016/j.mee.2015.04.041	journal	November 2015
Demonstration of wide frequency bandwidth electro-optic response in SBN thin film waveguide Gupta, Surbhi; Paliwal, Ayushi; Guo, Ruyan Optical Materials, Vol. 85 https://doi.org/10.1016/j.optmat.2018.08.008	journal	November 2018
Electrically tunable dielectric materials and strategies to improve their performances Kong, L. B.; Li, S.; Zhang, T. S. Progress in Materials Science, Vol. 55, Issue 8 https://doi.org/10.1016/j.pmatsci.2010.04.004	journal	November 2010
Si-Integrated BaTiO₃ for Electro-Optic Applications: Crystalline and Polarization Orientation Control Reynaud, Marc; Huyan, Huaixun; Du, Chaojie ACS Applied Electronic Materials, Vol. 5, Issue 8 https://doi.org/10.1021/acsaelm.3c00747	journal	August 2023
Polarization rotation mechanism for ultrahigh electromechanical response in single-crystal piezoelectrics Fu, Huaxiang; Cohen, Ronald E. Nature, Vol. 403, Issue 6767 https://doi.org/10.1038/35002022	journal	January 2000
Thermotropic phase boundaries in classic ferroelectrics Lummen, Tom T. A.; Gu, Yijia; Wang, Jianjun Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms4172	journal	January 2014
Large Pockels effect in micro- and nanostructured barium titanate integrated on silicon Abel, Stefan; Eltes, Felix; Ortmann, J. Elliott Nature Materials, Vol. 18, Issue 1 https://doi.org/10.1038/s41563-018-0208-0	journal	November 2018
An integrated optical modulator operating at cryogenic temperatures Eltes, Felix; Villarreal-Garcia, Gerardo E.; Caimi, Daniele Nature Materials, Vol. 19, Issue 11 https://doi.org/10.1038/s41563-020-0725-5	journal	July 2020
Barium titanate and lithium niobate permittivity and Pockels coefficients from megahertz to sub-terahertz frequencies Chelladurai, Daniel; Kohli, Manuel; Winiger, Joel Nature Materials, Vol. 24, Issue 6 https://doi.org/10.1038/s41563-025-02158-1	journal	March 2025
Hybrid integrated quantum photonic circuits Elshaari, Ali W.; Pernice, Wolfram; Srinivasan, Kartik Nature Photonics, Vol. 14, Issue 5 https://doi.org/10.1038/s41566-020-0609-x	journal	April 2020
Cryogenic optical data link for superconducting circuits Pintus, Paolo; Soltani, Mo; Moody, Galan Nature Photonics, Vol. 18, Issue 4 https://doi.org/10.1038/s41566-024-01417-y	journal	April 2024
Strong electro-optically active Ni-substituted Pb(Zr _0.35 Ti _0.65 )O ₃ thin films: toward integrated active and durable photonic devices Zhu, Minmin; Du, Zehui; Chng, Soon Siang Journal of Materials Chemistry C, Vol. 6, Issue 47 https://doi.org/10.1039/C8TC04576C	journal	January 2018
Relative dielectric constant of epitaxial BaTiO3 thin films in the GHz frequency range Hamano, T.; Towner, D. J.; Wessels, B. W. Applied Physics Letters, Vol. 83, Issue 25 https://doi.org/10.1063/1.1635967	journal	December 2003
Dispersion of Electro‐Optic Effect in BaTiO ₃ Johnston, Alan R. Journal of Applied Physics, Vol. 42, Issue 9 https://doi.org/10.1063/1.1660761	journal	August 1971
SOME DIELECTRIC AND ELECTRO‐OPTIC PROPERTIES OF BaTiO ₃ SINGLE CRYSTALS Johnson, C. J. Applied Physics Letters, Vol. 7, Issue 8 https://doi.org/10.1063/1.1754387	journal	October 1965
A phenomenological thermodynamic potential for BaTiO3 single crystals Li, Y. L.; Cross, L. E.; Chen, L. Q. Journal of Applied Physics, Vol. 98, Issue 6 https://doi.org/10.1063/1.2042528	journal	September 2005
Ultrawide range dielectric spectroscopy of BaTiO3-based perovskite dielectrics Tsurumi, T.; Li, J.; Hoshina, T. Applied Physics Letters, Vol. 91, Issue 18 https://doi.org/10.1063/1.2804570	journal	October 2007
The effect of grain and particle size on the microwave properties of barium titanate (BaTiO3) McNeal, Mark P.; Jang, Sei-Joo; Newnham, Robert E. Journal of Applied Physics, Vol. 83, Issue 6 https://doi.org/10.1063/1.367097	journal	March 1998
Trapped-ion quantum computing: Progress and challenges Bruzewicz, Colin D.; Chiaverini, John; McConnell, Robert Applied Physics Reviews, Vol. 6, Issue 2 https://doi.org/10.1063/1.5088164	journal	June 2019
Large impact of strain on the electro-optic effect in (Ba, Sr)TiO3 thin films: Experiment and theoretical comparison Kondo, Shinya; Yamada, Tomoaki; Tagantsev, Alexander K. Applied Physics Letters, Vol. 115, Issue 9 https://doi.org/10.1063/1.5117218	journal	August 2019
Materials for emergent silicon-integrated optical computing Demkov, Alexander A.; Bajaj, Chandrajit; Ekerdt, John G. Journal of Applied Physics, Vol. 130, Issue 7 https://doi.org/10.1063/5.0056441	journal	August 2021
Strong electro-optic effect in Mg incorporated ZnO thin films Yuan, X.; Yamada, T.; Meng, L. Applied Physics Letters, Vol. 121, Issue 15 https://doi.org/10.1063/5.0103831	journal	October 2022
Giant electro-optic response in transparent rhombohedral ferroelectric Sm-PIN-PMN-PT crystal based on domain engineering Wen, Yiyang; Ren, Hongda; Du, Xiaona Journal of Applied Physics, Vol. 136, Issue 11 https://doi.org/10.1063/5.0230598	journal	September 2024
Low-temperature growth of epitaxial BaTiO3 thin films with significant electro-optic coefficients Cao, Yilin; Wen, Yiyang; Yang, Yongtao Applied Physics Letters, Vol. 126, Issue 11 https://doi.org/10.1063/5.0237644	journal	March 2025
Domain wall scattering determining the transmittance of transparent ferroelectric crystals Xiong, Zixiang; Zhu, Jian; Ma, Jiaxin Applied Physics Letters, Vol. 126, Issue 19 https://doi.org/10.1063/5.0260262	journal	May 2025
Thickness dependence of the electro-optic properties in epitaxial Hf0.5Zr0.5O2 thin films: Evident response down to 3 nm Dastgir, Afeefa; Yuan, Xueyou; Shen, Yufan Applied Physics Letters, Vol. 126, Issue 24 https://doi.org/10.1063/5.0267559	journal	June 2025
High frequency dielectric relaxation in BaTio₃derived materials Kazaoui, S.; Ravez, J.; Elissalde, C. Ferroelectrics, Vol. 135, Issue 1 https://doi.org/10.1080/00150199208230015	journal	October 1992
Bridging phases at the morphotropic boundaries of lead oxide solid solutions Noheda, B.; Cox, D. E. Phase Transitions, Vol. 79, Issue 1-2 https://doi.org/10.1080/01411590500467262	journal	January 2006
Dielectric Constant in Perovskite Type Crystals Barrett, John H. Physical Review, Vol. 86, Issue 1 https://doi.org/10.1103/PhysRev.86.118	journal	April 1952
On-chip microwave-to-optical quantum coherent converter based on a superconducting resonator coupled to an electro-optic microresonator Javerzac-Galy, C.; Plekhanov, K.; Bernier, N. R. Physical Review A, Vol. 94, Issue 5 https://doi.org/10.1103/PhysRevA.94.053815	journal	November 2016
Thermodynamic theory of linear optical and electro-optical properties of ferroelectrics Ross, Aiden; Ali, Mohamed S. M. M.; Saha, Akash Physical Review B, Vol. 111, Issue 8 https://doi.org/10.1103/PhysRevB.111.085109	journal	February 2025
Dielectric, elastic, piezoelectric, electro-optic, and elasto-optic tensors of BaTiO 3 crystals Zgonik, M.; Bernasconi, P.; Duelli, M. Physical Review B, Vol. 50, Issue 9 https://doi.org/10.1103/PhysRevB.50.5941	journal	September 1994
Monoclinic and triclinic phases in higher-order Devonshire theory Vanderbilt, David; Cohen, Morrel H. Physical Review B, Vol. 63, Issue 9 https://doi.org/10.1103/PhysRevB.63.094108	journal	January 2001
Origin of the High Piezoelectric Response in PbZr 1 − x Ti x O 3 Guo, R.; Cross, L. E.; Park, S-E. Physical Review Letters, Vol. 84, Issue 23 https://doi.org/10.1103/PhysRevLett.84.5423	journal	June 2000
Ferroelectric soft mode and microwave dielectric relaxation in BaTiO3−PbMg1/3Nb2/3O3 ceramics Bovtun, V.; Nuzhnyy, D.; Kempa, M. Physical Review Materials, Vol. 5, Issue 1 https://doi.org/10.1103/PhysRevMaterials.5.014404	journal	January 2021
Microwaves in Quantum Computing Bardin, Joseph C.; Slichter, Daniel H.; Reilly, David J. IEEE Journal of Microwaves, Vol. 1, Issue 1 https://doi.org/10.1109/JMW.2020.3034071	journal	January 2021
Effect of Uniaxial Stress Upon the Electromechanical Properties of Various Piezoelectric Ceramics and Single Crystals Viehland, D. Journal of the American Ceramic Society, Vol. 89, Issue 3 https://doi.org/10.1111/j.1551-2916.2005.00879.x	journal	March 2006
Probing Ferroelectrics Using Optical Second Harmonic Generation Denev, Sava A.; Lummen, Tom T. A.; Barnes, Eftihia Journal of the American Ceramic Society, Vol. 94, Issue 9 https://doi.org/10.1111/j.1551-2916.2011.04740.x	journal	August 2011
Epitaxial integration of BaTiO3 on Si for electro-optic applications Guo, Wei; Posadas, Agham B.; Demkov, Alexander A. Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 39, Issue 3 https://doi.org/10.1116/6.0000923	journal	April 2021
Blueprint for a microwave trapped ion quantum computer Lekitsch, Bjoern; Weidt, Sebastian; Fowler, Austin G. Science Advances, Vol. 3, Issue 2 https://doi.org/10.1126/sciadv.1601540	journal	February 2017
Superconducting Qubits: Current State of Play Kjaergaard, Morten; Schwartz, Mollie E.; Braumüller, Jochen Annual Review of Condensed Matter Physics, Vol. 11, Issue 1 https://doi.org/10.1146/annurev-conmatphys-031119-050605	journal	March 2020
Recent Advances in Nonlinear Optical and Electro-Optical Materials Chen, Chuang-tian; Liu, Guang-zhao Annual Review of Materials Science, Vol. 16, Issue 1 https://doi.org/10.1146/annurev.ms.16.080186.001223	journal	August 1986
Indications of Two Separate Relaxators in the Subphonon Region of Tetragonal BaTiO ₃ Laabidi, K.; Fontana, M. D.; Maglione, M. Europhysics Letters (EPL), Vol. 26, Issue 4 https://doi.org/10.1209/0295-5075/26/4/012	journal	May 1994
Barium titanate (BaTiO_3) RF characterization for application in electro-optic modulators Rosa, Alvaro; Tulli, Domenico; Castera, Pau Optical Materials Express, Vol. 7, Issue 12 https://doi.org/10.1364/OME.7.004328	journal	November 2017
Electrooptic modulation up to 40 GHz in a barium titanate thin film waveguide modulator Tang, Pingsheng; Towner, D. J.; Hamano, T. Optics Express, Vol. 12, Issue 24 https://doi.org/10.1364/OPEX.12.005962	journal	January 2004
Ultralow voltage, high-speed, and energy-efficient cryogenic electro-optic modulator Pintus, Paolo; Singh, Anshuman; Xie, Weiqiang Optica, Vol. 9, Issue 10 https://doi.org/10.1364/OPTICA.463722	journal	October 2022
Molecular Mechanisms in Smart Materials Newnham, Robert E. MRS Bulletin, Vol. 22, Issue 5 https://doi.org/10.1557/S0883769400033170	journal	May 1997
Linear electro-optic effect in ferroelectric HfO₂-based epitaxial thin films Kondo, Shinya; Shimura, Reijiro; Teranishi, Takashi Japanese Journal of Applied Physics, Vol. 60, Issue 7 https://doi.org/10.35848/1347-4065/ac087d	journal	June 2021
Effect of Ni doping on the electro-optic property in K(Ta _0.6 Nb _0.4 )O ₃ films Yuan, Xueyou; Sakurai, Yuji; Kondo, Shinya Japanese Journal of Applied Physics, Vol. 61, Issue SN https://doi.org/10.35848/1347-4065/ac7ea9	journal	July 2022

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barium titanate
electro-optic effect
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Title: Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO3 Thin Films

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Title: Colossal Cryogenic Electro‐Optic Response Through Metastability in Strained BaTiO₃ Thin Films