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Self-assembled quantum dots in a nanowire system for quantum photonics

Nature Materials volume 12, pages 439–444 (2013)Cite this article

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Abstract

Quantum dots embedded within nanowires represent one of the most promising technologies for applications in quantum photonics. Whereas the top-down fabrication of such structures remains a technological challenge, their bottom-up fabrication through self-assembly is a potentially more powerful strategy. However, present approaches often yield quantum dots with large optical linewidths, making reproducibility of their physical properties difficult. We present a versatile quantum-dot-in-nanowire system that reproducibly self-assembles in core–shell GaAs/AlGaAs nanowires. The quantum dots form at the apex of a GaAs/AlGaAs interface, are highly stable, and can be positioned with nanometre precision relative to the nanowire centre. Unusually, their emission is blue-shifted relative to the lowest energy continuum states of the GaAs core. Large-scale electronic structure calculations show that the origin of the optical transitions lies in quantum confinement due to Al-rich barriers. By emitting in the red and self-assembling on silicon substrates, these quantum dots could therefore become building blocks for solid-state lighting devices and third-generation solar cells.

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Figure 1: Schematics of the quantum-dot-in-nanowire system.
Figure 2: Structure of quantum-dots-in-a-nanowire.
Figure 3: Cathodoluminescence of a single nanowire.
Figure 4: Photoluminescence of a quantum-dot-in-nanowire system.
Figure 5: Atomistic calculations of electronic states in a quantum-dot- in-nanowire system.

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References

  1. Shields, A. J. Semiconductor quantum light sources. Nature Photon. 1, 215–223 (2007).

    Article  CAS  Google Scholar 

  2. Borgstrom, M. T., Zwiller, V., Muller, E. & Imamoglu, A. Optically bright quantum dots in single nanowires. Nano Lett. 5, 1439–1443 (2005).

    Article  Google Scholar 

  3. Claudon, J. et al. A highly efficient single-photon source based on a quantum dot in a photonic nanowire. Nature Photon. 4, 174–177 (2010).

    Article  CAS  Google Scholar 

  4. Bulgarini, G. et al. Spontaneous emission control of single quantum dots in bottom-up nanowire waveguides. Appl. Phys. Lett. 100, 121106 (2012).

    Article  Google Scholar 

  5. Reimer, M. E. et al. Bright single-photon sources in bottom-up tailored nanowires. Nature Commun. 3, 737 (2012).

    Article  Google Scholar 

  6. Heinrich, J. et al. Single photon emission from positioned GaAs/AlGaAs photonic nanowires. Appl. Phys. Lett. 96, 211117 (2010).

    Article  Google Scholar 

  7. Uccelli, E., Arbiol, J., Morante, J. R. & Fontcuberta i Morral, A. InAs quantum dot arrays decorating the facets of GaAs nanowires. ACS Nano 4, 5985–5993 (2010).

    Article  CAS  Google Scholar 

  8. Bounouar, S. et al. Ultrafast room temperature single-photon source from nanowire-quantum dots. Nano Lett. 12, 2977–2981 (2012).

    Article  CAS  Google Scholar 

  9. Agarwal, R. & Lieber, C. M. Semiconductor nanowires: Optics and optoelectronics. Appl. Phys. A 85, 209–215 (2006).

    Article  CAS  Google Scholar 

  10. Kelzenberg, M. D. et al. Enhanced absorption and carrier collection in Si wire arrays for photovoltaic applications. Nature Mater. 9, 239–244 (2010).

    Article  CAS  Google Scholar 

  11. Moreau, E. et al. Single-mode solid-state single photon source based on isolated quantum dots in pillar microcavities. Appl. Phys. Lett. 79, 2865–2867 (2001).

    Article  CAS  Google Scholar 

  12. Moskalenko, E. S., Larsson, M., Schoenfeld, W. V., Petroff, P. M. & Holtz, P. O. Carrier transport in self-organized InAs/GaAs quantum-dot structures studied by single-dot spectroscopy. Phys. Rev. B 73, 155336 (2006).

    Article  Google Scholar 

  13. Dalgarno, P. A. et al. Hole recapture limited single photon generation from a single n-type charge-tunable quantum dot. Appl. Phys. Lett. 92, 193103 (2008).

    Article  Google Scholar 

  14. Colombo, C., Spirkoska, D., Frimmer, M., Abstreiter, G. & Fontcuberta i Morral, A. Ga-assisted catalyst-free growth mechanism of GaAs nanowires by molecular beam epitaxy. Phys. Rev. B 77, 155326 (2008).

    Article  Google Scholar 

  15. Heigoldt, M. et al. Long range epitaxial growth of prismatic heterostructures on the facets of catalyst-free GaAs nanowires. J. Mater. Chem. 19, 840–848 (2009).

    Article  CAS  Google Scholar 

  16. Fontcuberta i Morral, A. et al. Prismatic quantum heterostructures synthesized on molecular-beam epitaxy GaAs nanowires. Small 4, 899–903 (2008).

    Article  CAS  Google Scholar 

  17. Biasiol, G. & Kapon, E. Mechanisms of self-ordering of quantum nanostructures grown on nonplanar surfaces. Phys. Rev. Lett. 81, 2962–2965 (1998).

    Article  CAS  Google Scholar 

  18. Biasiol, G., Gustafsson, A., Leifer, K. & Kapon, E. Mechanisms of self-ordering in nonplanar epitaxy of semiconductor nanostructures. Phys. Rev. B 65, 205306 (2002).

    Article  Google Scholar 

  19. Steinke, L. et al. Nanometer-scale sharpness in corner-overgrown heterostructures. Appl. Phys. Lett. 93, 193117 (2008).

    Article  Google Scholar 

  20. Skold, N. et al. Phase segregation in AlInP shells on GaAs nanowires. Nano Lett. 6, 2743–2747 (2006).

    Article  Google Scholar 

  21. Dalgarno, P. A. et al. Coulomb interactions in single charged self-assembled quantum dots: Radiative lifetime and recombination energy. Phys. Rev. B 77, 245311 (2008).

    Article  Google Scholar 

  22. Wang, L. W. & Zunger, A. Linear combination of bulk bands method for large-scale electronic structure calculations on strained nanostructures. Phys. Rev. B 59, 15806–15818 (1999).

    Article  CAS  Google Scholar 

  23. Franceschetti, A., Fu, H., Wang, L. W. & Zunger, A. Many-body pseudopotential theory of excitons in InP and CdSe quantum dots. Phys. Rev. B 60, 1819–1829 (1999).

    Article  CAS  Google Scholar 

  24. Colombo, C., Heiß, M., Grätzel, M. & Fontcuberta i Morral, A. Gallium arsenide p-i-n radial structures for photovoltaic applications. Appl. Phys. Lett. 94, 173108 (2009).

    Article  Google Scholar 

  25. Bjork, M. T. et al. Few-electron quantum dots in nanowires. Nano Lett. 4, 1621–1625 (2004).

    Article  Google Scholar 

  26. Hayden, O., Agarwal, R. & Lieber, C. M. Nanoscale avalanche photodiodes for highly sensitive and spatially resolved photon detection. Nature Mater. 5, 352–356 (2006).

    Article  CAS  Google Scholar 

  27. Van Weert, M. H. M. et al. Selective excitation and detection of spin states in a single nanowire quantum dot. Nano Lett. 9, 1989–1993 (2009).

    Article  CAS  Google Scholar 

  28. Witek, B. J. et al. Measurement of the g-factor tensor in a quantum dot and disentanglement of exciton spins. Phys. Rev. B 84, 195305 (2011).

    Article  Google Scholar 

  29. Bernal, S. et al. The interpretation of HREM images of supported metal catalysts using image simulation: profile view images. Ultramicroscopy 72, 135–164 (1998).

    Article  CAS  Google Scholar 

  30. Arbiol, J. et al. Optimization of tin dioxide nanosticks faceting for the improvement of palladium nanocluster epitaxy. Appl. Phys. Lett. 80, 329–331 (2002).

    Article  CAS  Google Scholar 

  31. Heiss, M. et al. Catalyst-free nanowires with axial InxGa1−xAs/GaAs heterostructures. Nanotechnology 20, 075603 (2009).

    Article  Google Scholar 

  32. Luo, J.-W., Bester, G. & Zunger, A. Atomistic pseudopotential calculations of thickness-fluctuation GaAs quantum dots. Phys. Rev. B 79, 125329 (2009).

    Article  Google Scholar 

  33. Wang, L. W. & Zunger, A. Solving Schrodinger’s equation around a desired energy—Application to silicon quantum dots. J. Chem. Phys. 100, 2394–2397 (1994).

    Article  CAS  Google Scholar 

  34. Bowler, D. R. & Miyazaki, T. O(N) methods in electronic structure calculations. Rep. Prog. Phys. 75, 036503 (2012).

    Article  CAS  Google Scholar 

  35. Skylaris, C. K., Haynes, P. D., Mostofi, A. A. & Payne, M. C. Introducing ONETEP: Linear-scaling density functional simulations on parallel computers. J. Chem. Phys. 122, 084119 (2005).

    Article  Google Scholar 

  36. Hine, N. D. M., Haynes, P. D., Mostofi, A. A. & Payne, M. C. Linear-scaling density-functional simulations of charged point defects in Al2O3 using hierarchical sparse matrix algebra. J. Chem. Phys. 133, 114111 (2010).

    Article  CAS  Google Scholar 

  37. Hine, N. D. M., Haynes, P. D., Mostofi, A. A., Skylaris, C-K. & Payne, M. C. Linear-scaling density-functional theory with tens of thousands of atoms: Expanding the scope and scale of calculations with ONETEP. Comput. Phys. Commun. 180, 1041–1053 (2009).

    Article  CAS  Google Scholar 

  38. Avraam, P. W., Hine, N. D. M., Tangney, P. & Haynes, P. D. Fermi-level pinning can determine polarity in semiconductor nanorods. Phys. Rev. B 85, 115404 (2012).

    Article  Google Scholar 

  39. O’Regan, D. D., Payne, M. C. & Mostofi, A. A. Generalized Wannier functions: A comparison of molecular electric dipole polarizabilities. Phys. Rev. B 85, 193101 (2012).

    Article  Google Scholar 

  40. Perdew, J. P. & Zunger, A. Self-interaction correction to density-functional approximations for many-electron systems. Phys. Rev. B 23, 5048–5079 (1981).

    Article  CAS  Google Scholar 

  41. Momma, K. & Izumi, F. VESTA 3 for three-dimensional visualization of crystal, volumetric and morphology data. J. Appl. Crystallogr. 44, 1272–1276 (2011).

    Article  CAS  Google Scholar 

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Acknowledgements

A.F.i.M. acknowledges funding from ERC through the UpCon grant and SNF through Grant No. 134506. Both A.F.i.M. and R.J.W. acknowledge support from NCCR QSIT. The Phantoms Foundation is acknowledged for sponsoring B.K.’s visit to Lund University. This work was supported by the Spanish MICINN Projects MAT2010-15138, CSD2009-00013 and CSD2009-00050. J.A. and J.R.M. acknowledge Generalitat de Catalunya 2009-SGR-770, NanoAraCat and XaRMAE and European RDF support. The authors acknowledge F. J. Belarre for the making of the TEM cross-sections; A.G. thanks L. Samuelson and the Swedish Research Council for support. D.D.O. acknowledges N. D. M. Hine and the ONETEP developers’ group for discussions and software support, and the EPFL HPC service for generous provision of computing resources. The work carried out by J.W.L. and A.Z. was funded by the US Department of Energy, Office of Science, Basic Energy Science, Materials Sciences and Engineering under contract number DE-AC36-08GO28308 to NREL and CU Boulder.

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Author notes

  1. M. Heiss and Y. Fontana: These authors contributed equally to this work

Authors and Affiliations

  1. Laboratoire des Matériaux Semiconducteurs, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland

    M. Heiss, Y. Fontana, B. Ketterer, S. Conesa-Boj, E. Russo-Averchi & A. Fontcuberta i Morral

  2. Solid State Physics, The Nanometer Consortium, Lund University, Lund S-221 00, Box 118, Sweden

    A. Gustafsson

  3. Department of Physics, University of Basel, Klingelbergstrasse 82, CH4056 Basel, Switzerland

    G. Wüst, A. V. Kuhlmann, J. Houel & R. J. Warburton

  4. Instituto de Nanociencia de Aragon-ARAID and Departamento de Física de la Materia Condensada, Universidad de Zaragoza, 50018 Zaragoza, Spain

    C. Magen

  5. Theory and Simulation of Materials (THEOS), École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland

    D. D. O’Regan & N. Marzari

  6. National Renewable Energy Laboratory, Golden, Colorado 80401, USA

    J. W. Luo

  7. Catalonia Institute for Energy Research, IREC. 08930 Sant Adrià del Besòs, Spain

    J. R. Morante

  8. Department dÉlectrònica, Universitat de Barcelona, 08028 Barcelona, Spain

    J. R. Morante

  9. Interdisciplinary Center for Electron Microscopy, École Polytechnique Fédérale de Lausanne, 1015 Lausanne, Switzerland

    M. Cantoni

  10. Institució Catalana de Recerca i Estudis Avançats (ICREA) and Institut de Ciència de Materials de Barcelona, ICMAB-CSIC, E-08193 Bellaterra, CAT, Spain

    J. Arbiol

  11. University of Colorado, Boulder, Colorado 80309, USA

    A. Zunger

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  1. M. Heiss
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Contributions

M.H., E.R-A. and A.F.i.M. grew the samples. J.A., J.R.M. and C.M. performed HAADF STEM and EELS analysis. S.C-B. and M.C. mapped the composition of the quantum dots by EDX. J.A. and S.C-B. worked on the atomic modelling of the quantum dots. A.G. and B.K. measured the cathodoluminescence. M.H., Y.F., G.W., A.V.K., J.H. and R.J.W. participated in the optical spectroscopy studies. D.D.O. and N.M. performed density functional theory calculations. J.W.L. and A.Z. performed the empirical pseudopotential calculations. A.F.i.M. conceived and designed the experiments, and together with R.J.W., A.Z. and N.M. supervised the project. Y.F. made the figures and artwork. A.F.i.M., R.J.W., Y.F., A.Z., D.D.O., N.M. and J.A. wrote and edited the manuscript. All authors discussed the results and commented on the manuscript.

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Correspondence to M. Heiss or A. Fontcuberta i Morral.

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Heiss, M., Fontana, Y., Gustafsson, A. et al. Self-assembled quantum dots in a nanowire system for quantum photonics. Nature Mater 12, 439–444 (2013). https://doi.org/10.1038/nmat3557

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