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Structural effects of (111) growth of on and LSAT: New insights from 3D crystallographic characterization with 4D-STEM and digital dark field imaging
Phys. Rev. Materials 9, 123602 – Published 3 December, 2025
DOI: https://doi.org/10.1103/c3dm-7frg
Abstract
The three-dimensional orientation of La atom modulations has been mapped in two thin films of grown on and LSAT ([La,Sr,Al,Ta] oxide) using a 4D-scanning transmission electron microscopy method based on the recently developed Digital Dark Field method. This images the shifts of diffraction spots and the azimuthal intensity distribution in the First-Order Laue Zone, and then uses them to reconstruct and map the 3D crystallography. This clearly shows a flip from out-of-plane modulation with tensile strain on to in-plane modulation with compressive strain on LSAT. This hitherto unobserved crystallographic change had a significant influence on the out-of-plane lattice parameter which left more room for the full incorporation of the larger octahedra in the film grown on LSAT and therefore explained the improved Mn-Co ordering and better properties for this film. Moreover, the method would be applicable to many other systems of epitaxial growth of complex oxides, revealing crystallographic details of crucial importance to properties which are not visible in conventional atomic resolution imaging.
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New Insights into Functional Materials through Advanced Electron Microscopy
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References (57)
- A. C. Daykin and C. J. Kiely, Philos. Mag. A 68, 1331 (1993).
- I. MacLaren, Z. L. Wang, H. S. Wang, and Q. Li, Philos. Mag. A 82, 1405 (2002).
- I. MacLaren, R. Villaurrutia, and A. Peláiz-Barranco, J. Appl. Phys. 108, 034109 (2010).
- I. MacLaren, T. Ras, M. MacKenzie, A. J. Craven, D. W. McComb, and S. De Gendt, J. Electrochem. Soc. 156, G103 (2009).
- W. Y. Wang, Y. L. Zhu, Y. L. Tang, Y. B. Xu, Y. Liu, S. Li, S. R. Zhang, Y. J. Wang, and X. L. Ma, Appl. Phys. Lett. 109, 202904 (2016).
- J. C. Jiang, X. Q. Pan, and C. L. Chen, Appl. Phys. Lett. 72, 909 (1998).
- Y. L. Li, L. Q. Chen, G. Asayama, D. G. Schlom, M. A. Zurbuchen, and S. K. Streiffer, J. Appl. Phys. 95, 6332 (2004).
- S. Kitagawa, T. Ozaki, Y. Horibe, K. Yoshii, and S. Mori, Ferroelectrics 376, 122 (2008).
- C. J. Lu, Z. L. Wang, C. Kwon, and Q. X. Jia, J. Appl. Phys. 88, 4032 (2000).
- O. I. Lebedev, J. Verbeeck, G. V. Tendeloo, S. Amelinckx, F. S. Razavi, and H. U. Habermeier, Philos. Mag. A 81, 2865 (2001).
- C. L. Jia, S. B. Mi, K. Urban, I. Vrejoiu, M. Alexe, and D. Hesse, Nat. Mater. 7, 57 (2008).
- R. J. Zeches, M. D. Rossell, J. X. Zhang, A. J. Hatt, Q. He, C. H. Yang, A. Kumar, C. H. Wang, A. Melville, C. Adamo et al., Science 326, 977 (2009).
- C. T. Nelson, B. Winchester, Y. Zhang, S. J. Kim, A. Melville, C. Adamo, C. M. Folkman, S. H. Baek, C. B. Eom, D. G. Schlom et al., Nano Lett. 11, 828 (2011).
- H. W. Zandbergen, S. Freisem, T. Nojima, and J. Aarts, Phys. Rev. B 60, 10259 (1999).
- C. Ophus, Microsc. Microanal. 25, 563 (2019).
- I. MacLaren, T. A. Macgregor, C. S. Allen, and A. I. Kirkland, APL Mater. 8, 110901 (2020).
- B. H. Savitzky, S. E. Zeltmann, L. A. Hughes, H. G. Brown, S. Zhao, P. M. Pelz, T. C. Pekin, E. S. Barnard, J. Donohue, L. Rangel DaCosta et al., Microsc. Microanal. 27, 712 (2021).
- J. Tao, D. Niebieskikwiat, M. Varela, W. Luo, M. A. Schofield, Y. Zhu, M. B. Salamon, J. M. Zuo, S. T. Pantelides, and S. J. Pennycook, Phys. Rev. Lett. 103, 097202 (2009).
- E. F. Rauch and M. Véron, Eur. Phys. J. Appl. Phys. 66, 10701 (2014).
- V. B. Ozdol, C. Gammer, X. G. Jin, P. Ercius, C. Ophus, J. Ciston, and A. M. Minor, Appl. Phys. Lett. 106, 253107 (2015).
- Y. Meng and J.-M. Zuo, IUCrJ 3, 300 (2016).
- G. W. Paterson, R. W. H. Webster, A. Ross, K. A. Paton, T. A. Macgregor, D. McGrouther, I. MacLaren, and M. Nord, Microsc. Microanal. 26, 944 (2020).
- S. J. McCartan, I. Calisir, G. W. Paterson, R. W. H. Webster, T. A. Macgregor, D. A. Hall, and I. MacLaren, J. Am. Ceram. Soc. 104, 2388 (2021).
- C. Ophus, S. E. Zeltmann, A. Bruefach, A. Rakowski, B. H. Savitzky, A. M. Minor, and M. C. Scott, Microsc. Microanal. 28, 390 (2022).
- I. MacLaren, A. T. Fraser, M. R. Lipsett, and C. Ophus, Microsc. Microanal. 31, ozae104 (2025).
- Y. Cai, F. Phillipp, A. Zimmermann, L. Zhou, F. Aldinger, and A. Ruhle, Acta Mater. 51, 6429 (2003).
- Q. Qiao, S. Zhou, J. Tao, J.-C. Zheng, L. Wu, S. T. Ciocys, M. Iavarone, D. J. Srolovitz, G. Karapetrov, and Y. Zhu, Phys. Rev. Mater. 1, 054002 (2017).
- H. Wang, J. Gazquez, C. Frontera, M. F. Chisholm, A. Pomar, B. Martinez, and N. Mestres, NPG Asia Materials 11, 44 (2019).
- C. Meyer, V. Roddatis, P. Ksoll, B. Damaschke, and V. Moshnyaga, Phys. Rev. B 98, 134433 (2018).
- F. Lv, Y. Qin, Y. Gao, F. Huang, H. Tang, J. Liu, L. Long, and Y. Yang, Mater. Today Commun. 36, 106454 (2023).
- C. L. Bull, H. Y. Playford, K. S. Knight, G. B. G. Stenning, and M. G. Tucker, Phys. Rev. B 94, 014102 (2016).
- R. Egoavil, S. Hühn, M. Jungbauer, N. Gauquelin, A. Béché, G. Van Tendeloo, J. Verbeeck, and V. Moshnyaga, Nanoscale 7, 9835 (2015).
- S. Lv, Z. Wang, M. Saito, and Y. Ikuhara, J. Appl. Phys. 113, 203704 (2013).
- J. E. Kleibeuker, E.-M. Choi, E. D. Jones, T.-M. Yu, B. Sala, B. A. MacLaren, D. Kepaptsoglou, D. Hernandez-Maldonado, Q. M. Ramasse, L. Jones et al., NPG Asia Materials 9, e406 (2017).
- P. M. Jones, G. M. Rackham, and J. W. Steeds, Proc. R. Soc. London Ser. A 354, 197 (1977).
- J. P. Morniroli and A. Redjaimia, J. Microsc.-Oxf. 227, 157 (2007).
- J. C. H. Spence and C. Koch, Philos. Mag. B 81, 1701 (2001).
- F. T. Huang, A. Gloter, M. W. Chu, F. C. Chou, G. J. Shu, L. K. Liu, C. H. Chen, and C. Colliex, Phys. Rev. Lett. 105, 125502, (2010).
- M. Nord, J. Barthel, C. S. Allen, D. McGrouther, A. I. Kirkland, and I. MacLaren, Ultramicroscopy 226, 113296 (2021).
- M. Nord, A. Ross, D. McGrouther, J. Barthel, M. Moreau, I. Hallsteinsen, T. Tybell, and I. MacLaren, Phys. Rev. Mater. 3, 063605 (2019).
- A. Silinga, C. S. Allen, J. Barthel, C. Ophus, and I. MacLaren, Microsc. Microanal. 29, 1682 (2023).
- I. MacLaren, A. Silinga, J. Barthel, J. E. Kleibeuker, J. L. MacManus-Driscoll, C. S. Allen, and A. I. Kirkland, arXiv:2412.16297.
- I. Maclaren, A. Silinga, J. Barthel, J. Kleibeuker, J. L. MacManus-Driscoll, C. S. Allen, and A. I. Kirkland, Phys. Rev. Mater. 9, 094404 (2025).
- K. Kjaernes, I. Hallsteinsen, R. V. Chopdekar, M. Moreau, T. Bolstad, I. H. Svenum, S. M. Selbach, and T. Tybell, Phys. Rev. B 103, 224435 (2021).
- J. P. McCaffrey and J. M. Baribeau, Microsc. Res. Tech. 32, 449 (1995).
- I. MacLaren, A. T. Fraser, and M. R. Lipsett, The structural effects of (111) growth of on and LSAT–new insights from 3D crystallographic characterization with 4D-STEM and Digital Dark Field imaging, Enlighten Research Data (2025), https://researchdata.gla.ac.uk/2074/.
- A. Weickenmeier and H. Kohl, Acta Crystallogr. A 47, 590 (1991).
- H. Rose, Optik 45, 139 (1976).
- M. De Graef, Introduction to Conventional Transmission Electron Microscopy (Cambridge University Press, Cambridge, 2003).
- See Supplemental Material at http://link.aps.org/supplemental/10.1103/c3dm-7frg for investigations by simulation of the effects of thickness on the intensity distribution in the FOLZ for precession on and off, as well as calculations of SNR and SBR for one set of Digital Dark Field images.
- I. MacLaren, Z. L. Wang, H. S. Wang, and Q. Li, Appl. Phys. Lett. 80, 1406 (2002).
- D. T. L. Alexander, H. Meley, M. M. Schmitt, B. Mundet, J.-M. Triscone, P. Ghosez, and S. Gariglio, ACS Nano 19, 10126 (2025).
- C. L. Bull, D. Gleeson, and K. S. Knight, J. Phys.:Condens. Mat. 15, 4927 (2003).
- D. I. Woodward and I. M. Reaney, Acta Crystallogr. Sect. B 61, 387 (2005).
- E. F. Rauch, J. Portillo, S. Nicolopoulos, D. Bultreys, S. Rouvimov, and P. Moeck, Z. Krist.-Cryst. Mater. 225, 103 (2010).
- N. Cautaerts, P. Crout, H. W. Ånes, E. Prestat, J. Jeong, G. Dehm, and C. H. Liebscher, Ultramicroscopy 237, 113517 (2022).
- I. MacLaren, E. Frutos-Myro, S. Zeltmann, and C. Ophus, J. Microsc.-Oxf. 295, 131 (2024).