Hybrid Molecular Beam Epitaxy for Single-Crystalline Oxide Membranes with Binary Oxide Sacrificial Layers

Varshney, Shivasheesh; Choo, Sooho; Thompson, Liam; Yang, Zhifei; Shah, Jay; Wen, Jiaxuan; Koester, Steven J.; Mkhoyan, K. Andre; McLeod, Alexander S.; Jalan, Bharat

doi:10.1021/acsnano.3c11192

Title: Hybrid Molecular Beam Epitaxy for Single-Crystalline Oxide Membranes with Binary Oxide Sacrificial Layers

Journal Article · Mon Feb 05 00:00:00 EST 2024 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.3c11192· OSTI ID:2283938

Varshney, Shivasheesh ^[1]; Choo, Sooho ^[1]; Thompson, Liam ^[1]; Yang, Zhifei ^[1]; Shah, Jay ^[1]; Wen, Jiaxuan ^[1];

^[1];

^[1]; McLeod, Alexander S. ^[1];

^[1]

University of Minnesota, Twin Cities, MN (United States)

The advancement in thin-film exfoliation for synthesizing oxide membranes has led to possibilities for creating artificially assembled heterostructures with structurally and chemically incompatible materials. The sacrificial layer method is a promising approach to exfoliate as-grown films from a compatible material system, allowing for their integration with dissimilar materials. Nonetheless, the conventional sacrificial layers often possess an intricate stoichiometry, thereby constraining their practicality and adaptability, particularly when considering techniques such as molecular beam epitaxy (MBE). This is where easy-to-grow binary alkaline-earth-metal oxides with a rock salt crystal structure are useful. These oxides, which include (Mg, Ca, Sr, Ba)O, can be used as a sacrificial layer covering a much broader range of lattice parameters compared to conventional sacrificial layers and are easily dissolvable in deionized water. In this study, we show the epitaxial growth of the single-crystalline perovskite SrTiO₃ (STO) on sacrificial layers consisting of crystalline SrO, BaO, and Ba_1–xCa_xO films, employing a hybrid MBE method. Our results highlight the rapid (≤5 min) dissolution of the sacrificial layer when immersed in deionized water, facilitating the fabrication of millimeter-sized STO membranes. Using high-resolution X-ray diffraction, atomic-force microscopy, scanning transmission electron microscopy, impedance spectroscopy, and scattering-type near-field optical microscopy (SNOM), we demonstrate single-crystalline STO membranes with bulk-like intrinsic dielectric properties. Here, the employment of alkaline earth metal oxides as sacrificial layers is likely to simplify membrane synthesis, particularly with MBE, thus expanding the research and application possibilities.

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Research Organization:: University of Minnesota, Twin Cities, MN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR)

Grant/Contract Number:: SC0023464; SC0020211; FA9550-21-1-0025; FA9550-21-0460; FA9550-23-1-0247

OSTI ID:: 2283938

Journal Information:: ACS Nano, Vol. 18, Issue 8; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (63)

Freestanding complex-oxide membranes Pesquera, David; Fernández, Abel; Khestanova, Ekaterina Journal of Physics: Condensed Matter, Vol. 34, Issue 38 https://doi.org/10.1088/1361-648X/ac7dd5	journal	July 2022
Molecular beam epitaxy growth of epitaxial barium silicide, barium oxide, and barium titanate on silicon McKee, R. A.; Walker, F. J.; Conner, J. R. Applied Physics Letters, Vol. 59, Issue 7 https://doi.org/10.1063/1.105341	journal	August 1991
Phase transition enhanced superior elasticity in freestanding single-crystalline multiferroic BiFeO ₃ membranes Peng, Bin; Peng, Ren-Ci; Zhang, Yong-Qiang Science Advances, Vol. 6, Issue 34 https://doi.org/10.1126/sciadv.aba5847	journal	August 2020
Facile Chemical Route to Prepare Water Soluble Epitaxial Sr₃Al₂O₆ Sacrificial Layers for Free‐Standing Oxides Salles, Pol; Caño, Ivan; Guzman, Roger Advanced Materials Interfaces, Vol. 8, Issue 5 https://doi.org/10.1002/admi.202001643	journal	January 2021
Free‐standing microstructures of YBa ₂ Cu ₃ O _7−δ : A high‐temperature superconducting air bridge Lee, L. P.; Burns, M. J.; Char, K. Applied Physics Letters, Vol. 61, Issue 22 https://doi.org/10.1063/1.108092	journal	November 1992
Origami and materials science Liu, H.; Plucinsky, P.; Feng, F. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 379, Issue 2201 https://doi.org/10.1098/rsta.2020.0113	journal	May 2021
Synthesis of freestanding single-crystal perovskite films and heterostructures by etching of sacrificial water-soluble layers Lu, Di; Baek, David J.; Hong, Seung Sae Nature Materials, Vol. 15, Issue 12 https://doi.org/10.1038/nmat4749	journal	September 2016
Bendable Polycrystalline and Magnetic CoFe₂O₄ Membranes by Chemical Methods Salles, Pol; Guzmán, Roger; Zanders, David ACS Applied Materials & Interfaces, Vol. 14, Issue 10 https://doi.org/10.1021/acsami.1c24450	journal	March 2022
Elastic strain engineering of ferroic oxides Schlom, Darrell G.; Chen, Long-Qing; Fennie, Craig J. MRS Bulletin, Vol. 39, Issue 2 https://doi.org/10.1557/mrs.2014.1	journal	February 2014
Binary alkaline earth oxide mixtures: Estimation of the excess thermodynamic properties and calculation of the phase diagrams van der Kemp, W. J. M.; Blok, J. G.; van der Linde, P. R. Calphad, Vol. 18, Issue 3 https://doi.org/10.1016/0364-5916(94)90032-9	journal	July 1994
High Yield Transfer of Clean Large-Area Epitaxial Oxide Thin Films Zhang, Bowen; Yun, Chao; MacManus-Driscoll, Judith L. Nano-Micro Letters, Vol. 13, Issue 1 https://doi.org/10.1007/s40820-020-00573-4	journal	January 2021
Nanospectroscopy of Infrared Phonon Resonance Enables Local Quantification of Electronic Properties in Doped SrTiO ₃ Ceramics Lewin, Martin; Baeumer, Christoph; Gunkel, Felix Advanced Functional Materials, Vol. 28, Issue 42 https://doi.org/10.1002/adfm.201802834	journal	September 2018
Remote epitaxy Kim, Hyunseok; Chang, Celesta S.; Lee, Sangho Nature Reviews Methods Primers, Vol. 2, Issue 1 https://doi.org/10.1038/s43586-022-00122-w	journal	June 2022
Atomically precise interfaces from non-stoichiometric deposition Nie, Y. F.; Zhu, Y.; Lee, C. -H. Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms5530	journal	August 2014
Tuning Piezoelectricity via Thermal Annealing at a Freestanding Ferroelectric Membrane Han, Lu; Yang, Xinrui; Lun, Yingzhuo Nano Letters, Vol. 23, Issue 7 https://doi.org/10.1021/acs.nanolett.3c00096	journal	March 2023
3D architectures of single-crystalline complex oxides Kim, Shin-Ik; Choi, Hyung-Jin; Lee, Gwangyeob Materials Horizons, Vol. 7, Issue 6 https://doi.org/10.1039/D0MH00292E	journal	January 2020
Epitaxial Heusler Alloys: New Materials for Semiconductor Spintronics Palmstrøm, Chris MRS Bulletin, Vol. 28, Issue 10 https://doi.org/10.1557/mrs2003.213	journal	October 2003
Anomalous transport in high-mobility superconducting SrTiO ₃ thin films Yue, Jin; Ayino, Yilikal; Truttmann, Tristan K. Science Advances, Vol. 8, Issue 21 https://doi.org/10.1126/sciadv.abl5668	journal	May 2022
Stacking and Twisting of Freestanding Complex Oxide Thin Films Li, Ying; Xiang, Cheng; Chiabrera, Francesco M. Advanced Materials, Vol. 34, Issue 38 https://doi.org/10.1002/adma.202203187	journal	August 2022
Prominent Size Effects without a Depolarization Field Observed in Ultrathin Ferroelectric Oxide Membranes Sun, Haoying; Gu, Jiahui; Li, Yongqiang Physical Review Letters, Vol. 130, Issue 12 https://doi.org/10.1103/PhysRevLett.130.126801	journal	March 2023
Large magnetoelectric coupling in multiferroic oxide heterostructures assembled via epitaxial lift-off Pesquera, D.; Khestanova, E.; Ghidini, M. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16942-x	journal	June 2020
Sacrificial Water-Soluble BaO Layer for Fabricating Free-Standing Piezoelectric Membranes Takahashi, Ryota; Lippmaa, Mikk ACS Applied Materials & Interfaces, Vol. 12, Issue 22 https://doi.org/10.1021/acsami.0c05830	journal	May 2020
Significant Suppression of Cracks in Freestanding Perovskite Oxide Flexible Sheets Using a Capping Oxide Layer Gong, Lizhikun; Wei, Mian; Yu, Rui ACS Nano, Vol. 16, Issue 12 https://doi.org/10.1021/acsnano.2c08649	journal	November 2022
Free-standing epitaxial La1−x(Sr,Ca)xMnO3 membrane on Si for uncooled infrared microbolometer Kim, J. -H.; Grishin, A. M. Applied Physics Letters, Vol. 87, Issue 3 https://doi.org/10.1063/1.1996845	journal	July 2005
Model for quantitative tip-enhanced spectroscopy and the extraction of nanoscale-resolved optical constants McLeod, Alexander S.; Kelly, P.; Goldflam, M. D. Physical Review B, Vol. 90, Issue 8 https://doi.org/10.1103/PhysRevB.90.085136	journal	August 2014
Engineering the Electronic Structure of Graphene Zhan, Da; Yan, Jiaxu; Lai, Linfei Advanced Materials, Vol. 24, Issue 30 https://doi.org/10.1002/adma.201200011	journal	July 2012
Nonvolatile ferroelectric domain wall memory integrated on silicon Sun, Haoying; Wang, Jierong; Wang, Yushu Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-31763-w	journal	July 2022
Soft-Mode Phonons in SrTiO₃ Thin Films Studied by Far-Infrared Ellipsometry and Raman Scattering Sirenko, A. A.; Bernhard, C.; Golnik, A. MRS Proceedings, Vol. 603 https://doi.org/10.1557/PROC-603-245	journal	January 1999
A Fast Route Towards Freestanding Single-Crystalline Oxide Thin Films by Using YBa2Cu3O7-x as a Sacrificial Layer Chang, Yao-Wen; Wu, Ping-Chun; Yi, Jhih-Bang Nanoscale Research Letters, Vol. 15, Issue 1 https://doi.org/10.1186/s11671-020-03402-0	journal	August 2020
Freestanding crystalline oxide perovskites down to the monolayer limit Ji, Dianxiang; Cai, Songhua; Paudel, Tula R. Nature, Vol. 570, Issue 7759 https://doi.org/10.1038/s41586-019-1255-7	journal	June 2019
Epitaxial SrTiO ₃ films with dielectric constants exceeding 25,000 Yang, Zhifei; Lee, Dooyong; Yue, Jin Proceedings of the National Academy of Sciences, Vol. 119, Issue 23 https://doi.org/10.1073/pnas.2202189119	journal	June 2022
Large-lattice-parameter perovskite single-crystal substrates Uecker, Reinhard; Bertram, Rainer; Brützam, Mario Journal of Crystal Growth, Vol. 457 https://doi.org/10.1016/j.jcrysgro.2016.03.014	journal	January 2017
Transfer of Epitaxial SrTiO ₃ Nanothick Layers Using Water-Soluble Sacrificial Perovskite Oxides Bourlier, Yoan; Bérini, Bruno; Frégnaux, Mathieu ACS Applied Materials & Interfaces, Vol. 12, Issue 7 https://doi.org/10.1021/acsami.9b21047	journal	January 2020
Heterogeneous integration of single-crystalline complex-oxide membranes Kum, Hyun S.; Lee, Hyungwoo; Kim, Sungkyu Nature, Vol. 578, Issue 7793 https://doi.org/10.1038/s41586-020-1939-z	journal	February 2020
Synthesis of functional nitride membranes using sacrificial water-soluble BaO layers Chen, Shengru; Jin, Qiao; Lin, Shan Journal of Applied Physics, Vol. 133, Issue 4 https://doi.org/10.1063/5.0138633	journal	January 2023
Strain-induced room-temperature ferroelectricity in SrTiO3 membranes Xu, Ruijuan; Huang, Jiawei; Barnard, Edward S. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-16912-3	journal	June 2020
Crystalline Oxides on Silicon: The First Five Monolayers McKee, R. A.; Walker, F. J.; Chisholm, M. F. Physical Review Letters, Vol. 81, Issue 14 https://doi.org/10.1103/PhysRevLett.81.3014	journal	October 1998
Epitaxial optimization of atomically smooth Sr3Al2O6 for freestanding perovskite films by molecular beam epitaxy Sun, H. Y.; Zhang, C. C.; Song, J. M. Thin Solid Films, Vol. 697 https://doi.org/10.1016/j.tsf.2020.137815	journal	March 2020
Freestanding Perovskite Oxide Films: Synthesis, Challenges, and Properties Chiabrera, Francesco M.; Yun, Shinhee; Li, Ying Annalen der Physik, Vol. 534, Issue 9 https://doi.org/10.1002/andp.202200084	journal	June 2022
Novel synthesis approach for “stubborn” metals and metal oxides Nunn, William; Manjeshwar, Anusha Kamath; Yue, Jin Proceedings of the National Academy of Sciences, Vol. 118, Issue 32 https://doi.org/10.1073/pnas.2105713118	journal	August 2021
Growth of buried metal aluminides and gallides and of rare-earth monopnictides in compound semiconductors: a comparison Palmstrom, Chris J.; Sands, Tim D.; Harbison, James P. SPIE Proceedings https://doi.org/10.1117/12.20810	conference	October 1990
Freestanding epitaxial SrTiO ₃ nanomembranes via remote epitaxy using hybrid molecular beam epitaxy Yoon, Hyojin; Truttmann, Tristan K.; Liu, Fengdeng Science Advances, Vol. 8, Issue 51 https://doi.org/10.1126/sciadv.add5328	journal	December 2022
Towards a Large-Area Freestanding Single-Crystal Ferroelectric BaTiO3 Membrane Wang, Qixiang; Fang, Hong; Wang, Di Crystals, Vol. 10, Issue 9 https://doi.org/10.3390/cryst10090733	journal	August 2020
Enhanced polarization and abnormal flexural deformation in bent freestanding perovskite oxides Cai, Songhua; Lun, Yingzhuo; Ji, Dianxiang Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-32519-2	journal	August 2022
Solid-state miscibility gap and thermodynamics of the system BaO–SrO Jacob, K. T.; Varghese, Viji J. Mater. Chem., Vol. 5, Issue 7 https://doi.org/10.1039/JM9950501059	journal	January 1995
Nano-FTIR Absorption Spectroscopy of Molecular Fingerprints at 20 nm Spatial Resolution Huth, Florian; Govyadinov, Alexander; Amarie, Sergiu Nano Letters, Vol. 12, Issue 8 https://doi.org/10.1021/nl301159v	journal	July 2012
Van der Waals integration before and beyond two-dimensional materials Liu, Yuan; Huang, Yu; Duan, Xiangfeng Nature, Vol. 567, Issue 7748 https://doi.org/10.1038/s41586-019-1013-x	journal	March 2019
Giant Uniaxial Strain Ferroelectric Domain Tuning in Freestanding PbTiO ₃ Films Han, Lu; Fang, Yanhan; Zhao, Yunqi Advanced Materials Interfaces, Vol. 7, Issue 7 https://doi.org/10.1002/admi.201901604	journal	April 2020
A Generic Sacrificial Layer for Wide‐Range Freestanding Oxides with Modulated Magnetic Anisotropy Peng, Huining; Lu, Nianpeng; Yang, Shuzhen Advanced Functional Materials, Vol. 32, Issue 28 https://doi.org/10.1002/adfm.202111907	journal	April 2022
Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy Lee, J. H.; Luo, G.; Tung, I. C. Nature Materials, Vol. 13, Issue 9 https://doi.org/10.1038/nmat4039	journal	August 2014
Pseudoheterodyne detection for background-free near-field spectroscopy Ocelic, Nenad; Huber, Andreas; Hillenbrand, Rainer Applied Physics Letters, Vol. 89, Issue 10 https://doi.org/10.1063/1.2348781	journal	September 2006
Atomically flat single terminated oxide substrate surfaces Biswas, Abhijit; Yang, Chan-Ho; Ramesh, Ramamoorthy Progress in Surface Science, Vol. 92, Issue 2 https://doi.org/10.1016/j.progsurf.2017.05.001	journal	May 2017
On the Role of the Sr_3−xCa_xAl₂O₆ Sacrificial Layer Composition in Epitaxial La_0.7Sr_0.3MnO₃ Membranes Salles, Pol; Guzman, Roger; Barrera, Aleix Advanced Functional Materials, Vol. 33, Issue 41 https://doi.org/10.1002/adfm.202304059	journal	June 2023
c-axis oriented epitaxial BaTiO3 films on (001) Si Vaithyanathan, V.; Lettieri, J.; Tian, W. Journal of Applied Physics, Vol. 100, Issue 2 https://doi.org/10.1063/1.2203208	journal	July 2006
Single crystal functional oxides on silicon Bakaul, Saidur Rahman; Serrao, Claudy Rayan; Lee, Michelle Nature Communications, Vol. 7, Issue 1 https://doi.org/10.1038/ncomms10547	journal	February 2016
Phonon-enhanced light–matter interaction at the nanometre scale Hillenbrand, R.; Taubner, T.; Keilmann, F. Nature, Vol. 418, Issue 6894 https://doi.org/10.1038/nature00899	journal	July 2002
Infrared dispersion in SrTi $O_{3}$ at high temperature Servoin, J. L.; Luspin, Y.; Gervais, F. Physical Review B, Vol. 22, Issue 11 https://doi.org/10.1103/PhysRevB.22.5501	journal	December 1980
Large-Area Crystalline BaSnO ₃ Membranes with High Electron Mobilities Singh, Prastuti; Swartz, Adrian; Lu, Di ACS Applied Electronic Materials, Vol. 1, Issue 7 https://doi.org/10.1021/acsaelm.9b00215	journal	June 2019
A review of molecular-beam epitaxy of wide bandgap complex oxide semiconductors Nunn, William; Truttmann, Tristan K.; Jalan, Bharat Journal of Materials Research, Vol. 36, Issue 23 https://doi.org/10.1557/s43578-021-00377-1	journal	September 2021
Artifact free time resolved near-field spectroscopy Sternbach, A. J.; Hinton, J.; Slusar, T. Optics Express, Vol. 25, Issue 23 https://doi.org/10.1364/OE.25.028589	journal	January 2017
Beyond Substrates: Strain Engineering of Ferroelectric Membranes Pesquera, David; Parsonnet, Eric; Qualls, Alexander Advanced Materials, Vol. 32, Issue 43 https://doi.org/10.1002/adma.202003780	journal	September 2020
Extreme tensile strain states in La _0.7 Ca _0.3 MnO ₃ membranes Hong, Seung Sae; Gu, Mingqiang; Verma, Manish Science, Vol. 368, Issue 6486 https://doi.org/10.1126/science.aax9753	journal	April 2020
High-κ perovskite membranes as insulators for two-dimensional transistors Huang, Jing-Kai; Wan, Yi; Shi, Junjie Nature, Vol. 605, Issue 7909 https://doi.org/10.1038/s41586-022-04588-2	journal	May 2022

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