Interfacial atomic structure analysis at sub-angstrom resolution using aberration-corrected STEM
© Hsiao et al.; licensee Springer. 2014
Received: 20 June 2014
Accepted: 8 October 2014
Published: 17 October 2014
The atomic structure of a SiGe/Si epitaxial interface grown via molecular beam epitaxy on a single crystal silicon substrate was investigated using an aberration-corrected scanning transmittance electron microscope equipped with a high-angle annular dark-field detector and an energy-dispersive spectrometer. The accuracy required for compensation of the various residual aberration coefficients to achieve sub-angstrom resolution with the electron optics system was also evaluated. It was found that the interfacial layer was composed of a silicon single crystal, connected coherently to epitaxial SiGe nanolaminates. In addition, the distance between the dumbbell structures of the Si and Ge atoms was approximately 0.136 nm at the SiGe/Si interface in the  orientation. The corresponding fast Fourier transform exhibited a sub-angstrom scale point resolution of 0.78 Å. Furthermore, the relative positions of the atoms in the chemical composition line scan signals could be directly interpreted from the corresponding incoherent high-angle annular dark-field image.
KeywordsAberration correction HRTEM HRSTEM HAADF Z contrast EELS EDS
where A1, C1, A2, B2, C3, A3, and S3 are, respectively, the second-order astigmatism, defocus, third-order astigmatism, coma, spherical aberration (i.e., Cs), fourth-order astigmatism, and star aberration.
Recently developed aberration-corrected HRTEM [3, 4] and high-resolution scanning transmission electron microscopes (HRSTEM) improve the resolving power without the need to increase the electron beam energy [5–8]. Although still far from their ultimate diffraction limit, these instruments have been demonstrated to resolve sub-angstrom image features. HRSTEM high-angle annular dark-field (HAADF) imaging can be considered incoherent, thus nearly completely eliminating the diffraction and phase contrast. The contrast is then, to a good approximation, monotonic with thickness, and is also sensitive to changes in composition; for a typical geometry and material, it is approximately proportional to Z1.8, where Z is the atomic number. These properties also make the STEM HAADF signal ideal for recent tomography applications [9–11]. However, although many literature reports describe the instrumental details of how the aberration correctors are designed and function, the practical aberration correction for the atomic structure determination and interface analysis of functional materials is also important. On the other hand, the development of a device that can measure the distribution of all of the elements present in the material structure in order to monitor the success and quality of the process is required. To date, electron energy loss spectroscopy (EELS) [12, 13] and energy distribution spectroscopy (EDS) [14, 15] have been shown to be effective for measuring not only images of atoms but also chemical composition. The higher resolution provides much improved sensitivity for the atomic arrangements at defects and interfaces. Combining EDS with HRSTEM offers two advantages: inelastic interactions are always effectively local, such as in an incoherent HAADF image, and the inner shell ionization potential is as localized as possible for a given ionization edge. Consequently, the resulting incoherent image can be directly interpreted . In the present study, atomic resolution HRSTEM images of SiGe/Si interface were directly interpreted along with simultaneous chemical line scans based on detection of the incoherent signal using an aberration-corrected scanning transmission electron microscope.
Electropolished and chemically etched specimen of an epitaxial SiGe/Si semiconductor grown using molecular beam epitaxy (MBE) on a single crystal silicon  substrate was used in this study. An aberration-corrected STEM equipped with an HAADF detector and an EDS was used to analyze the atomic structure of each specimen (Titan 200 kV). Au-Pd bimetallic particles deposited on a thin amorphous carbon film was used as a reference for correcting the aberration coefficients of the electronic optics system. Because the aberrations were visible when the beam was tilted out of the optical axis, a series of images was acquired at different beam tilt angles . The aberration correction process was principally achieved by calculating the Zemlin tableau of a series of aberration coefficients followed by visualization of the phase shift image (phase plate). The required accuracy for compensation of the various residual aberration coefficients needed to achieve sub-angstrom resolution with the system was then determined. The probe forming aperture semiangle was 9.8 mrad, and the probe was focused to the size of 1 Å on the specimen with a beam current of 70 pA. The EDS was used to detect the chemical element distribution of the SiGe/Si interface. In this method, a coherent focused probe was scanned across the specimen, and the resultant x-ray emission spectrum was recorded at each probe position. These spectra were then used to construct an elemental line scan. The acquisition time for a single x-ray spectrum was 20 s.
Results and discussion
According to this calculation, the influence of the various axial aberrations on the shape and even more importantly on the electron intensity distribution within the probe could be evaluated .
For aberration correction, improvement in the transfer function was directly seen in the ronchigram, a diffraction pattern of an amorphous film obtained using a large convergence angle that gives a direct image of the aberration function χ(θ, φ). In the present aberration corrected system, there was a large uniform region at the center of the ronchigram. The range of minimum contrast at the center defined an area of constant electron phase that was appropriate for use in forming a small probe. By allowing higher convergence angles, the beam intensity also increased, which is important for chemical analysis.
The atomic resolution imaging and spectroscopic analysis of an SiGe/Si interface grown via molecular beam epitaxy was investigated using aberration-corrected HRSTEM. The phase plates were calculated from the aberration coefficients of the measured probe tableau for various outer tilt angle of the optical axis, and the accuracy required for the compensation of the various residual aberration coefficients in order to achieve sub-angstrom resolution with the electron optics system was evaluated. The HRSTEM HAADF dumbbell image revealed that the distance between the Si and Ge atoms was approximately 1.36 Å, and the corresponding fast Fourier transform confirmed a point resolution on the sub-angstrom scale (0.78 Å). In addition, the experimental results demonstrated that complementary EDS line scan signals could be directly correlated to the atomic-resolution HAADF image.
The authors gratefully acknowledge financially support from the Ministry of Science and Technology, Taiwan (contract no. 103-2622-E-492 -011 -CC3).
- Scherzer O: Über einige Fehler von Elektronenlinsen. Zeitschrift für Physik 1936, 101(9):593–603.View ArticleGoogle Scholar
- Scherzer O: Sphärische und chromatische Korrektur von Elektronenlinsen. Optik 1947, 2: 114–132.Google Scholar
- Haider M, Uhlemann S, Schwan E, Rose H, Kabius B, Urban K: Electron microscopy image enhanced. Nature 1998, 392: 768–769. 10.1038/33823View ArticleGoogle Scholar
- Uhlemann S, Haider M: Residual wave aberrations in the first spherical aberration corrected transmission electron microscope. Ultramicroscopy 1998, 72: 109–119. 10.1016/S0304-3991(97)00102-2View ArticleGoogle Scholar
- Krivanek OL, Dellby N, Lupini AR: Towards sub-Å electron beams. Ultramicroscopy 1999, 78: 1–11. 10.1016/S0304-3991(99)00013-3View ArticleGoogle Scholar
- Haider M, Uhlemann S, Zach J: Upper limits for the residual aberrations of a high-resolution aberration-corrected STEM. Ultramicroscopy 2000, 81: 163–175. 10.1016/S0304-3991(99)00194-1View ArticleGoogle Scholar
- Batson PE, Dellby N, Krivanek OL: Sub-angstrom resolution using aberration-corrected electron optics. Nature 2000, 418: 617–620.View ArticleGoogle Scholar
- Nellist PD, Chisholm MF, Dellby N, Krivanek OL, Murfitt MF, Szilagyi ZS, Lupini AR, Borisevich A, Sides WH Jr, Pennycook SJ: Direct sub-angstrom imaging of a crystal lattice. Science 2004, 305: 1741–1741. 10.1126/science.1100965View ArticleGoogle Scholar
- Midgley PA, EDunin-Borkowski R: Electron tomography and holography in materials science. Nature Mater 2009, 8: 271–280. 10.1038/nmat2406View ArticleGoogle Scholar
- Van Aert S, Batenburg KJ, Rossell MD, Erni R, van Tendeloo G: Three dimensional atomic imaging of crystalline nanoparticles. Nature 2011, 470: 374–377. 10.1038/nature09741View ArticleGoogle Scholar
- Chen CC, Zhu C, White ER, Chiu CY, Scott MC, Regan BC, Marks LD, Huang Y, Miao J: Three-dimensional imaging of dislocations in a nanoparticle at atomic resolution. Nature 2013, 496: 74–77. 10.1038/nature12009View ArticleGoogle Scholar
- Urban KW: Studying atomic structures by aberration-corrected transmission electron microscopy. Science 2008, 321: 506–510. 10.1126/science.1152800View ArticleGoogle Scholar
- Muller D: Structure and bonding at the atomic scale by scanning transmission electron microscopy. Nat Mater 2009, 8: 263–270. 10.1038/nmat2380View ArticleGoogle Scholar
- Chu M-W, Liou SC, Chang C-P, Choa F-S, Chen CH: Emergent chemical mapping at atomic-column resolution by energy-dispersive X-ray spectroscopy in an aberration-corrected electron microscope. Phys Rev Lett 2010, 104: 196101–196104.View ArticleGoogle Scholar
- D’Alfonso AJ, Freitag B, Klenov D, Allen LJ: Atomic-resolution chemical mapping using energy-dispersive x-ray spectroscopy. Phys Rev B 2010, 81: 100101. 1–4 1–4View ArticleGoogle Scholar
- O'Keefe MA: Seeing atoms with aberration-corrected sub-angstrom electron microscopy. Ultramicroscopy 2008, 108: 196–209. 10.1016/j.ultramic.2007.07.009View ArticleGoogle Scholar
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