Mapping Polar Distortions using Nanobeam Electron Diffraction and a Cepstral Approach
Source abstract
Abstract
Abstract Measuring local polar ordering is key to understanding ferroelectricity in thin films, especially for systems with small domains or significant disorder. Scanning nanobeam electron diffraction (NBED) provides an effective local probe of lattice parameters, local fields, polarization directions, and charge densities, which can be analyzed using a relatively low beam dose over large fields of view. However, quantitatively extracting the magnitudes and directions of polarization vectors from NBED remains challenging. Here, we use a cepstral approach, similar to a pair distribution function, to determine local polar displacements that drive ferroelectricity from NBED patterns. Because polar distortions generate asymmetry in the diffraction pattern intensity, we can efficiently recover the underlying displacements from the imaginary part of the cepstrum transform. We investigate the limits of this technique using analytical and simulated data and give experimental examples, achieving the order of 1.1 pm precision and mapping of polar displacements with nanometer resolution.
Source: crossref · Quality: baseline
Research context
OpenAlex topics: Surface and Thin Film Phenomena · Advanced Electron Microscopy Techniques and Applications · Electron and X-Ray Spectroscopy Techniques
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Material Measurement Laboratory, National Institute of Standards and Technology , 100 Bureau Drive, Gaithersburg, MD 20899 , USA
School of Applied and Engineering Physics, Cornell University , 142 Sciences Drive, Ithaca, NY 14853 , USA
Department of Metallurgical and Materials Engineering, Colorado School of Mines , 1301 19th Street, Golden, CO 80401 , USA
Funding
U.S. National Institute of Standards and Technology · NSF MRSEC · NSF Cooperative · NSF MRI
References (71)
Show source-provided references
1. Atomic level observation of octahedral distortions at the perovskite oxide heterointerface10.1038/srep02214 ↗
2. Nature and evolution of incommensurate charge order in manganites visualized with cryogenic scanning transmission electron microscopy10.1073/pnas.1714901115 ↗
3. The problem with determining atomic structure at the nanoscale10.1126/science.1135080 ↗
4. Phase dependence of Kikuchi patterns. I. Theory10.1107/S0108767388009304 ↗
5. Mapping octahedral tilts and polarization across a domain wall in BiFeO3 from Z-contrast scanning transmission electron microscopy image atomic column shape analysis10.1021/nn1011539 ↗
6. Influence of lens aberrations, specimen thickness and tilt on differential phase contrast STEM images10.1016/j.ultramic.2020.113118 ↗
7. Atomic-resolution differential phase contrast STEM on ferroelectric materials: A mean-field approach10.1103/PhysRevB.101.184116 ↗
8. Flexoelectric rotation of polarization in ferroelectric thin films10.1038/nmat3141 ↗
9. Atomically resolved mapping of polarization and electric fields across ferroelectric/oxide interfaces by Z-contrast imaging10.1002/adma.201004641 ↗
10. Electron ptychography achieves atomic-resolution limits set by lattice vibrations10.1126/science.abg2533 ↗
11. Visibility of single atoms10.1126/science.168.3937.1338 ↗
12. Imaging polarity in two dimensional materials by breaking Friedel's law10.1016/j.ultramic.2020.113019 ↗
13. Egerton · 201110.1007/978-1-4419-9583-4 ↗
14. Local atomic order and hierarchical polar nanoregions in a classical relaxor ferroelectric10.1038/s41467-019-10665-4 ↗
15. Advancing reverse Monte Carlo structure refinements to the nanoscale10.1107/S1600576717013140 ↗
16. Using EBSD and TEM-Kikuchi patterns to study local crystallography at the domain boundaries of lead zirconate titanate10.1111/j.1365-2818.2008.02004.x ↗
17. Robust atomic resolution imaging of light elements using scanning transmission electron microscopy10.1063/1.3265946 ↗
18. Interface-induced nonswitchable domains in ferroelectric thin films10.1038/ncomms5693 ↗
19. Holtz · 2022
20. Dimensionality-induced change in topological order in multiferroic oxide superlattices10.1103/PhysRevLett.126.157601 ↗
21. Topological defects in hexagonal manganites: Inner structure and emergent electrostatics10.1021/acs.nanolett.7b01288 ↗
22. Atomic lattice disorder in charge-density-wave phases of exfoliated dichalcogenides (1T-TaS 2)10.1073/pnas.1606044113 ↗
23. Howie · 1971 · 27510.1016/B978-0-12-780584-9.50014-3 ↗
24. Image contrast and localized signal selection techniques10.1111/j.1365-2818.1979.tb00228.x ↗
25. Diffraction contrast of electron microscope images of crystal lattice defects—II. The development of a dynamical theory
26. Multislice formula for inclined illumination10.1107/S0567739482001594 ↗
27. Atomic-scale study of electric dipoles near charged and uncharged domain walls in ferroelectric films10.1038/nmat2080 ↗
28. Unit-cell scale mapping of ferroelectricity and tetragonality in epitaxial ultrathin ferroelectric films10.1038/nmat1808 ↗
29. Local crystal structure analysis with several picometer precision using scanning transmission electron microscopy10.1016/j.ultramic.2009.11.014 ↗
30. Kirkland · 202010.1007/978-3-030-33260-0 ↗
31. Simulation of annular dark field stem images using a modified multislice method10.1016/0304-3991(87)90229-4 ↗
32. Atomic-resolution electron microscopy of nanoscale local structure in lead-based relaxor ferroelectrics10.1038/s41563-020-0794-5 ↗
33. Ferroelectric domain walls in PbTiO3 are effective regulators of heat flow at room temperature10.1021/acs.nanolett.9b02991 ↗
34. Phase contrast STEM for thin samples: Integrated differential phase contrast10.1016/j.ultramic.2015.10.011 ↗
35. Quantitative comparisons of contrast in experimental and simulated bright-field scanning transmission electron microscopy images10.1103/PhysRevB.80.174106 ↗
36. Determining ferroelectric polarity at the nanoscale10.1063/1.3549300 ↗
37. Enhanced energy storage with polar vortices in ferroelectric nanocomposites10.1103/PhysRevApplied.8.034014 ↗
38. Experimental measurement of stress at a four-domain junction in lead zirconate titanate10.1063/1.1886910 ↗
39. On the origin of differential phase contrast at a locally charged and globally charge-compensated domain boundary in a polar-ordered material10.1016/j.ultramic.2015.03.016 ↗
40. Local stabilisation of polar order at charged antiphase boundaries in antiferroelectric (Bi 0.85 Nd 0.15)(Ti 0.1 Fe 0.9)O 310.1063/1.4818002 ↗
41. EELS log-ratio technique for specimen-thickness measurement in the TEM10.1002/jemt.1060080206 ↗
42. On the breakdown of Friedel's law in electron backscattering channelling patterns10.1107/S0108767388004532 ↗
43. Friedel's law in the dynamical theory of diffraction10.1107/S0365110X55001023 ↗
44. Room design for high-performance electron microscopy10.1016/j.ultramic.2006.04.017 ↗
45. Discovery of stable skyrmionic state in ferroelectric nanocomposites10.1038/ncomms9542 ↗
46. Unusual phase transitions in ferroelectric nanodisks and nanorods10.1038/nature03107 ↗
47. Spontaneous vortex nanodomain arrays at ferroelectric heterointerfaces10.1021/nl1041808 ↗
48. Four-dimensional scanning transmission electron microscopy (4D-STEM): From scanning nanodiffraction to ptychography and beyond10.1017/S1431927619000497 ↗
49. The exit-wave power-cepstrum transform for scanning nanobeam electron diffraction: Robust strain mapping at subnanometer resolution and subpicometer precision10.1016/j.ultramic.2020.112994 ↗
50. A Fourier series method for the determination of the components of interatomic distances in crystals10.1103/PhysRev.46.372 ↗
51. Reimer · 2008
52. Domains in ferroelectric nanodots10.1021/nl901661a ↗
53. Crystal structure refinement of AlN and GaN10.1016/0038-1098(77)90959-0 ↗
54. Friedel's law in electron diffraction as applied to the study of domain structures in non-centrosymmetrical crystals10.1002/pssb.2220580127 ↗
55. Emergent chirality in a polar meron to skyrmion phase transition10.1038/s41467-023-36950-x ↗
56. On the accurate measurement of structure-factor amplitudes and phases by electron diffraction10.1107/S0108767392005087 ↗
57. Spence · 201310.1093/acprof:oso/9780199668632.001.0001 ↗
58. Atomistic structure of 90° domain walls in ferroelectric PbTiO 3 thin films10.1080/01418619508244477 ↗
59. Domain configurations in ferroelectric PbTiO3 thin films: The influence of substrate and film thickness10.1016/0167-2738(94)00151-H ↗
60. Contrast of 180° domains of PbTiO3 in an electron microscopic image. Acta Crystallographica Section A: Crystal Physics, Diffraction
61. High dynamic range pixel array detector for scanning transmission electron microscopy10.1017/S1431927615015664 ↗
62. Refinement of crystal structural parameters using two-dimensional energy-filtered CBED patterns10.1107/S0108767399005401 ↗
63. Two-dimensional mapping of polarizations of rhombohedral nanostructures in the tetragonal phase of BaTiO 3 by the combined use of the scanning transmission electron microscopy and convergent-beam electron diffraction methods10.1063/1.4819221 ↗
64. Atomic-scale imaging of individual dopant atoms and clusters in highly n-type bulk Si10.1038/416826a ↗
65. Direct observations of ferroelectric domains in lithium niobate10.1002/pssb.19680260221 ↗
66. Strain-induced room-temperature ferroelectricity in SrTiO3 membranes10.1038/s41467-020-16912-3 ↗
67. Observation of polar vortices in oxide superlattices10.1038/nature16463 ↗
68. Spatially resolved steady-state negative capacitance10.1038/s41586-018-0855-y ↗
69. Effects of interface dislocations on properties of ferroelectric thin films10.1016/j.jmps.2007.01.011 ↗
70. Sample tilt effects on atom column position determination in ABF–STEM imaging10.1016/j.ultramic.2015.10.008 ↗
71. Zuo · 201710.1007/978-1-4939-6607-3 ↗