Skip to main content Accessibility help

Simultaneous Quantification of Indium and Nitrogen Concentration in InGaNAs Using HAADF-STEM

  • Tim Grieb (a1), Knut Müller (a1), Emmanuel Cadel (a2), Andreas Beyer (a3), Marco Schowalter (a1), Etienne Talbot (a2), Kerstin Volz (a3) and Andreas Rosenauer (a1)...


To unambiguously evaluate the indium and nitrogen concentrations in In x Ga1−x N y As1−y , two independent sources of information must be obtained experimentally. Based on high-resolution scanning transmission electron microscopy (STEM) images taken with a high-angle annular dark-field (HAADF) detector the strain state of the InGaNAs quantum well is determined as well as its characteristic HAADF-scattering intensity. The strain state is evaluated by applying elasticity theory and the HAADF intensity is used for a comparison with multislice simulations. The combination of both allows for determination of the chemical composition where the results are in accordance with X-ray diffraction measurements, three-dimensional atom probe tomography, and further transmission electron microscopy analysis. The HAADF-STEM evaluation was used to investigate the influence of As-stabilized annealing on the InGaNAs/GaAs sample. Photoluminescence measurements show an annealing-induced blue shift of the emission wavelength. The chemical analysis precludes an elemental diffusion as origin of the energy shift—instead the results are in agreement with a model based on an annealing-induced redistribution of the atomic next-neighbor configuration.


Corresponding author

* Corresponding author.


Hide All
Albrecht, M., Grillo, V., Remmele, T., Strunk, H.P., Egorov, A.Y., Dumitras, G., Riechert, H., Kaschner, A., Heitz, R. & Hoffmann, A. (2002). Effect of annealing on the In and N distribution in InGaAsN quantum wells. Appl Phys Lett 81(15), 27192721.
Buyanova, I.A., Pozina, G., Hai, P.N., Thinh, N.Q., Bergman, J.P., Chen, W.M., Xin, H.P. & Tu, C.W. (2000). Mechanism for rapid thermal annealing improvements in undoped GaN x As1−x /GaAs structures grown by molecular beam epitaxy. Appl Phys Lett 77, 23252327.
Carlino, E. (2010). Quantitative Z-contrast atomic resolution studies of semiconductor nanostructured materials. J Phys Conf Ser 209, 012005.
Forbes, B.D., Martin, A.V., Findlay, S.D., D’Alfonso, A.J. & Allen, L.J. (2010). Quantum mechanical model for phonon excitation in electron diffraction and imaging using a Born-Oppenheimer approximation. Phys Rev B 82, 104103.
Friedman, D.J., Geisz, J.F., Kurtz, S.R. & Olson, J.M. (1998). 1-Ev solar cells with GaInNAs active layer. J Cryst Growth 195, 409415.
Glas, F. (2004). The effect of the static atomic displacements on the structure factors of weak reflections in cubic semiconductor alloys. Philos Mag 84(20), 20552074.
Grieb, T., Müller, K., Fritz, R., Grillo, V., Schowalter, M., Volz, K. & Rosenauer, A. (2013). Quantitative chemical evaluation of dilute GaNAs using ADF STEM: Avoiding surface strain induced artifacts. Ultramicroscopy 129, 19.
Grieb, T., Müller, K., Fritz, R., Schowalter, M., Neugebohrn, N., Knaub, N., Volz, K. & Rosenauer, A. (2012). Determination of nitrogen concentration in dilute GaNAs by STEM HAADF Z-contrast imaging and STEM-HAADF strain state analysis. Ultramicroscopy 117, 1523.
Grillo, V. (2009). The effect of surface strain relaxation on HAADF imaging. Ultramicroscopy 109, 14531464.
Grillo, V., Albrecht, M., Remmele, T., Strunk, H.P., Egorov, A.Y. & Riechert, H. (2001). Simultaneous experimental evaluation of In and N concentrations in InGaAsN quantum wells. J Appl Phys 90(8), 37923798.
Grillo, V., Carlino, E. & Glas, F. (2008). Influence of the static atomic displacement on atomic resolution Z-contrast imaging. Phys Rev B 77, 054103.
Grillo, V. & Rossi, F. (2011). A new insight on crystalline strain and defect features by STEM-ADF imaging. J Cryst Growth 318, 11511156.
Keating, P.N. (1966). Effect of invariance requirements on the elastic strain energy of crystals with application to the diamond structure. Phys Rev 145(2), 637645.
Kim, K. & Zunger, A. (2001). Spatial correlations in GaInAsN alloys and their effects on band-gap enhancement and electron localization. Phys Rev Lett 86, 26092612.
Kitatani, T., Nakahara, K., Kondow, M., Uomi, K. & Tanaka, T. (2000). Mechanism analysis of improved GaInNAs optical properties through thermal annealing. J Cryst Growth 209, 345349.
Klar, P.J., Grüning, H., Koch, J., Schäfer, S., Volz, K., Stolz, W., Heimbrodt, W., Kamal Saadi, A.M., Lindsay, A. & O’Reilly, E.P. (2001). (Ga, In)(N, As)-fine structure of the band gap due to nearest-neighbor configurations of the isovalent nitrogen. Phys Rev B 64(12), 121203.
Kondow, M., Kitatani, T., Nakatsuka, S., Larson, M.C., Nakahara, K., Yazawa, Y., Okai, M. & Uomi, K. (1997). GaInNAs: A novel material for long-wavelength semiconductor lasers. IEEE J Sel Topics Quantum Electron 3, 719730.
Kurtz, S., Webb, J., Gedvilas, L., Friedmann, D., Geisz, J., Olson, J., King, R., Joslin, D. & Karam, N. (2001). Structural changes during annealing of GaInAsN. Appl Phys Lett 78, 748750.
LeBeau, J. & Stemmer, S. (2008). Experimental quantification of annular dark-field images in scanning transmission electron microscopy. Ultramicroscopy 108, 16531658.
Litvinov, D., Gerthsen, D., Rosenauer, A., Hetterich, M., Grau, A., Gilet, P. & Grenouillet, L. (2004). Determination of the nitrogen distribution in InGaNAs/GaAs quantum wells by transmission electron microscopy. Appl Phys Lett 85, 37433745.
Mehrtens, T., Bley, S., Satyam, P.V. & Rosenauer, A. (2012). Optimization of the preparation of GaN-based specimens with low-energy ion milling for (S)TEM. Micron 43, 902909.
Molina, S.I., Sales, D.L., Galindo, P.L., Fuster, D., González, Y., Alén, B., González, L., Varela, M. & Pennycook, S.J. (2009). Column-by-column compositional mapping by Z-contrast imaging. Ultramicroscopy 109, 172176.
Müller, K., Schowalter, M., Rosenauer, A., Hu, D., Schaadt, D.M., Hetterich, M., Gilet, P., Rubel, O., Fritz, R. & Volz, K. (2011). Atomic scale annealing effects of In x Ga1−x N y As1−y studied by TEM three-beam imaging. Phys Rev B 84, 045316.
Müller, K., Schowalter, M., Rosenauer, A., Rubel, O. & Volz, K. (2010). Effect of bonding and static atomic displacements on composition quantification in In x Ga1−x N y As1−y . Phys Rev B 81(7), 075315.
Nellist, P. & Rodenburg, J. (1994). Beyond the conventional information limit: The relevant coherence function. Ultramicroscopy 54, 6174.
Plimpton, S. (1995). Fast parallel algorithms for short-range molecular dynamics. J Comput Phys 117, 119.
Riechert, H., Ramakrishnan, A. & Steinle, G. (2002). Development of InGaAsN-based 1.3 μm VCSELs. Semicond Sci Technol 17, 892897.
Riley, J., Bernal, R., Li, Q., Espinosa, H., Wang, G. & Lauhon, L. (2012). Atom probe tomography of a-axis GaN nanowires: Analysis of nonstoichiometric evaporation behavior. ACS Nano 6, 38983906.
Rosenauer, A., Fischer, U., Gerthsen, D. & Förster, A. (1998). Composition evaluation by lattice fringe analysis. Ultramicroscopy 72, 121133.
Rosenauer, A., Gries, K., Müller, K., Pretorius, A., Schowalter, M., Avramescu, A., Engl, K. & Lutgen, S. (2009). Measurement of specimen thickness and composition in Al x Ga1−x N/GaN using high-angle annular dark field images. Ultramicroscopy 109, 11711182.
Rosenauer, A., Mehrtens, T., Müller, K., Gries, K., Schowalter, M., Satyam, P.V., Bley, S., Tessarek, C., Hommel, D., Sebald, K., Seyfried, M., Gutowski, J., Avramescu, A., Engl, K. & Lutgen, S. (2011). Composition mapping in InGaN by scanning transmission electron microscopy. Ultramicroscopy 111, 13161327.
Rosenauer, A. & Schowalter, M. (2007). STEMSIM – A new software tool for simulation of STEM HAADF Z-contrast imaging. Springer Proc Phys 120, 169172.
Rosenauer, A., Schowalter, M., Glas, F. & Lamoen, D. (2005). First-principles calculations of 002 structure factors for electron scattering in strained In x Ga1−x As. Phys Rev B 72, 085326.
Saxey, D. (2011). Correlated ion analysis and the interpretation of atom probe mass spectra. Ultramicroscopy 111, 473479.
Schowalter, M., Müller, K. & Rosenauer, A. (2012). Scattering amplitudes and static atomic correction factors for the composition-sensitive 002 reflection in sphalerite ternary iii-v and ii-vi semiconductors. Acta Cryst A 68, 6876.
Schowalter, M., Rosenauer, A., Titantah, J.T. & Lamoen, D. (2009). Computation and parametrization of the temperature dependence of Debye-Waller factors for group iv, iii-v and ii-vi semiconductors. Acta Cryst A 65, 517.
Scott, J., Docherty, F.T., MacKenzie, M., Smith, W., Miller, B., Collins, C.L. & Craven, A.J. (2006). Sample preparation for nanoanalytical electron microscopy using the FIB lift-out method and low energy ion milling. J Phys Conf Ser 26, 223226.
Spruytte, S.G., Larson, M.C., Wampler, W., Coldren, C.W., Petersen, H.E. & Harris, J.S. (2001). Nitrogen incorporation in group iii-nitride-arsenide materials grown by elemental source molecular beam epitaxy. J Cryst Growth 227–228, 506515.
Thompson, K., Lawrence, D., Larson, D.J., Olson, J.D., Kelly, T.F. & Gorman, B. (2007). In situ site-specific specimen preparation for atom probe tomography. Ultramicroscopy 107, 131139.
Van Dyck, D. (2009). Is the frozen phonon model adequate to describe inelastic phonon scattering? Ultramicroscopy 109, 677682.
Volz, K., Torunski, T., Kunert, B., Rubel, O., Nau, S., Reinhard, S. & Stolz, W. (2004). Specific structural and compositional properties of (GaIn)(NAs) and their influence on optoelectronic device performance. J Cryst Growth 272, 739747.
Volz, K., Torunski, T., Rubel, O. & Stolz, W. (2008). Direct structural evidence of the change in n-iii bonding in (GaIn)(NAs) before and after thermal annealing. J Appl Phys 104, 053504.
Vurgaftman, I., Meyer, J.R. & Ram-Mohan, L.R. (2001). Band parameters for iii-v compound semiconductors and their alloys. J Appl Phys 89(11), 58155875.
Wagner, J., Geppert, T., Küohler, K., Ganser, P. & Maier, M. (2003). Bonding of nitrogen in dilute GaInAsN and AlGaAsN studied by Raman spectroscopy. Solid State Electron 47, 461465.
Wang, Z. (1998). The “frozen-lattice” approach for incoherent phonon excitation in electron scattering. How accurate is it? Acta Cryst A 54, 460467.
Wang, Z. (2003). Thermal diffuse scattering in sub-angstrom quantitative electron microscopy – Phenomenon, effects and approaches. Micron 34, 141155.
Weickenmeier, A. & Kohl, H. (1991). Computation of absorptive form factors for high-energy electron diffraction. Acta Cryst A 47(5), 590597.


Related content

Powered by UNSILO

Simultaneous Quantification of Indium and Nitrogen Concentration in InGaNAs Using HAADF-STEM

  • Tim Grieb (a1), Knut Müller (a1), Emmanuel Cadel (a2), Andreas Beyer (a3), Marco Schowalter (a1), Etienne Talbot (a2), Kerstin Volz (a3) and Andreas Rosenauer (a1)...


Full text views

Total number of HTML views: 0
Total number of PDF views: 0 *
Loading metrics...

Abstract views

Total abstract views: 0 *
Loading metrics...

* Views captured on Cambridge Core between <date>. This data will be updated every 24 hours.

Usage data cannot currently be displayed.