The influence of temperature on the photoluminescence properties of single InAs quantum dots grown on patterned GaAs

  • Juha Tommila1Email author,

    Affiliated with

    • Christian Strelow2,

      Affiliated with

      • Andreas Schramm1,

        Affiliated with

        • Teemu V Hakkarainen1,

          Affiliated with

          • Mihail Dumitrescu1,

            Affiliated with

            • Tobias Kipp2 and

              Affiliated with

              • Mircea Guina1

                Affiliated with

                Nanoscale Research Letters20127:313

                DOI: 10.1186/1556-276X-7-313

                Received: 4 May 2012

                Accepted: 6 June 2012

                Published: 19 June 2012


                We report the temperature-dependent photoluminescence of single site-controlled and self-assembled InAs quantum dots. We have used nanoimprint lithography for patterning GaAs(100) templates and molecular beam epitaxy for quantum dot deposition. We show that the influence of the temperature on the photoluminescence properties is similar for quantum dots on etched nanopatterns and randomly positioned quantum dots on planar surfaces. The photoluminescence properties indicate that the prepatterning does not degrade the radiative recombination rate for the site-controlled quantum dots.


                III-V semiconductors InAs Quantum dots Site-controlled quantum dots Molecular beam epitaxy Nanoimprint lithography 78, optical properties, condensed-matter spectroscopy and other interactions of radiation and particles with condensed matter 78.67.-n, optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures 78.67.Hc, quantum dots


                Single semiconductor quantum dots (QDs) are the building blocks for future information processing platforms, such as quantum cryptography and quantum computing [13]. QDs have been exploited as single [4, 5] and entangled photon sources [6, 7]. In order to enable such applications, the QDs should be fabricated at well-defined positions, rendering impractical the standard epitaxial processes that would result in randomly positioned QDs. The control of QD position can be achieved by creating preferential nucleation sites via patterning the deposited surface. Site-controlled quantum dots (SCQDs) have been fabricated utilizing various patterning techniques [812] combined with molecular beam epitaxy (MBE) or metalorganic vapor phase epitaxy. The optical properties of single QDs are easily deteriorated by defects, which are induced during the patterning and subsequent overgrowth. The defects cause nonradiative recombination channels, which degrade the QD photoluminescence (PL). Measuring the optical properties of a QD as a function of temperature provides a method to assess the quality of the QDs.

                In this paper, we study the temperature-dependent PL of single SCQDs fabricated on a nanoimprint lithography patterned GaAs(100) surface. We compare their PL properties to the ones of single self-assembled quantum dots (SAQDs) grown on unpatterned surface.


                The InAs QD sample was fabricated on a GaAs(100) substrate by combination of MBE and soft ultraviolet nanoimprint lithography (UV-NIL). First, a GaAs buffer layer, an AlGaAs barrier layer and a GaAs layer were grown by MBE. Second, the sample was patterned ex situ by UV-NIL using mr-UVCur06 (Micro Resist Technology GmbH, Berlin, Germany) as an etch mask and an EVG-620 (EV Group, St. Florian am Inn, Austria) mask aligner. The patterned area consisted of holes with a diameter of 100 nm arranged in a square lattice with the period of 1.5 μm. After patterning, the sample was chemically cleaned, and the native oxides were removed using IPA-, HCl-, and NH4OH-based solutions. The process is described in more detail in [13]. After chemical treatment, the sample was loaded into the MBE reactor, and a 30-nm GaAs buffer layer was grown at 470°C. Growth-interrupted MBE [13, 14] at 540°C was used to form single SCQDs in the patterned holes and low density SAQDs randomly positioned outside the patterned area. Finally, the QDs were capped by 20 and 50 nm of GaAs grown at 540°C and at 590°C, respectively, and 50-nm AlGaAs grown at 590°C. The structure was finished by a 10-nm GaAs layer.

                Micro-PL (μPL) measurements were performed at various temperatures up to 70 K using a continuous-wave laser emitting at 532 nm for excitation and a microscope objective (numerical aperture = 0.8) for diffraction-limited laser beam focusing and PL light collection. The PL signal was dispersed by a 50-cm spectrometer containing a 1,200 lines/mm grating and detected by a cooled Si CCD camera. The spectral resolution of the setup was 66 μeV.

                Results and discussion

                In order to evaluate the large scale optical quality of the sample, we added a diverging lens into the beam of the excitation laser in the μPL setup. The widened illumination field had a diameter of about 30 μm on the sample. Figure 1 shows PL intensity images from the edge of the patterned area within the spectral range of 850 to 1,000 nm at temperatures of 5, 40, and 70 K. Regularly spaced (1.5-μm period) bright spots illustrate PL emission from single SCQDs. Spots outside the array originate from SAQDs. For the lowest temperature (Figure 1a), the whole PL image is affected by a relatively strong background. Spectrally resolved measurements confirm its origin in the wetting layer (WL) emission, which is typical for low density QDs [15]. At low temperatures, the photoexcited carriers are trapped and recombined in the WL at localizing potentials induced by irregularities in WL [16]. The effect was confirmed by the fine structure of the WL PL (not shown). At 40 K (measurement shown in Figure 1b), the emission from WL is reduced because of the thermal escape of the carriers from the localizing potentials and a very thin WL typical for this growth technique [17]. An array of intense PL spots from the single SCQDs with 1.5-μm period is observed. When the sample was heated up to 70 K (measurement shown in Figure 1c), the PL emission from some individual QDs decreased due to thermal escape of carriers from the QD states and decreased carrier population in the WL acting as a carrier reservoir for QDs [16]. In spite of the slight deviations in uniformity, most of the SCQDs exhibit bright luminescence even at relatively high temperatures, indicating a low amount of nonradiative recombination processes.
                Figure 1

                PL intensity images from the edge of the patterned area. Intensity within the spectral range of 850 to 1,000 nm was measured at temperatures of 5 K (a), 40 K (b), and 70 K (c). The excitation power and wavelength were 1.77 μW and 532 nm, respectively.

                Further on, we performed μPL measurements with focused excitation within a temperature range of 5 to 70 K for randomly selected bright SCQDs within the pattern as well as for SAQDs outside the patterned area. Figure 2a,b shows typical sets of single QD emission spectra of a SCQD and a SAQD, respectively, at temperatures from 5 to 70 K. At high temperatures, only single exciton (X)-related peaks are visible in the spectrum, whereas at lower temperatures, also emission from biexciton and charged exciton states is observed. Figure 3 shows the peak energies of the exciton transitions (marked with X in Figure 2) for SCQD and SAQD as a function of temperature. The energies obey the temperature dependency of the InAs band gap energy as obtained by Varshni's law (solid lines), which is shifted in energy [1820]. The integrated intensities of the single exciton PL for SCQD and SAQD are shown in the inset of Figure 3. The increase in intensity around 50 K is attributed to the increased amount of carriers transferred to the QD from the WL [16]. Figure 4 shows the linewidth of the exciton transition as a function of temperature calculated from Lorentzian fits to the exciton peak. The exciton linewidths for SCQD and SAQD show very similar temperature dependencies. At low temperatures, i.e., 5 to 30 K, the linewidth appears to be limited by the spectral resolution of 66 μeV of the measurement setup, but it increases rapidly to 250 μeV when increasing the temperature from 40 to 70 K. The linewidth broadening is mainly caused by phonon scattering [21] and is in good agreement with previous results for SAQDs [22] and SCQDs [23, 24].
                Figure 2

                Single QD emission spectra for SCQD (a) and SAQD (b) at temperatures 5 to 70 K. The spectra are vertically shifted for clarity. The excitation power was 2 nW.

                Figure 3

                Peak energies of the exciton (X) transitions as a function of temperature. Solid lines indicate the slope of the temperature dependency of the InAs band gap energy obtained by Varshni's law. The parameters are α = 0.27 meV/K and β = 135 K. The inset shows the integrated PL intensities of the exciton transitions.

                Figure 4

                Linewidths of the exciton transitions as a function of temperature. The linewidths are obtained from Lorentzian fits to the exciton peak. Error bars indicate the error of Lorentzian fits.


                We have studied the influence of temperature on the PL properties of single site-controlled InAs QDs fabricated by a combination of soft UV-NIL and MBE. We have shown that the QDs in etched holes emitting at 945 nm have temperature-dependent PL properties similar to the self-assembled QDs grown on planar surface. The PL properties indicate that the defects induced by the patterning do not degrade significantly the emission of the site-controlled QDs. Thus, soft UV-NIL-positioned QDs are considerable candidates for fabricating large-scale optoelectronic devices.



                Molecular beam epitaxy






                Quantum dot


                Self-assembled quantum dot


                Site-controlled quantum dot


                Ultraviolet nanoimprint lithography


                Wetting layer


                Single exciton.



                The research was carried out within the Academy of Finland project DAUNTLESS (decision number 123951). JT acknowledges the National Doctoral Programme in Nanoscience (NGS-NANO), the Vilho, Yrjö and Kalle Väisälä Foundation and the Industrial Research Fund at Tampere University of Technology (Tuula and Yrjö Neuvo fund) for the financial support. AS acknowledges funding from the Academy of Finland within the project 138940. TVH acknowledges financial support from the Finnish National Graduate School in Materials Physics, Jenny and Antti Wihuri Foundation, and Finnish Foundation for Technology Promotion. CS and TK acknowledge funding from the Deutsche Forschungsgemeinschaft via project KI 1257/1.

                Authors’ Affiliations

                Optoelectronics Research Centre, Tampere University of Technology
                Institute of Physical Chemistry, University of Hamburg


                1. Waks E, Inoue K, Santori C, Fattal D, Vuckovic J, Solomon GS, Yamamoto Y: Quantum cryptography with a single photon turnstile. Nature 2002, 420: 762. 10.1038/420762aView Article
                2. Santori C, Fattal D, Vuckovic J, Solomon GS, Yamamoto Y: Indistinguishable photons from a single-photon device. Nature 2002, 419: 594–597. 10.1038/nature01086View Article
                3. Knill E, Laflamme R, Milburn GJ: A scheme for efficient quantum computation with linear optics. Nature 2001, 409: 46–52. 10.1038/35051009View Article
                4. Michler P, Kiraz A, Becher C, Schoenfeld WV, Petroff PM, Zhang L, Hu E, Imamogùlu A: A quantum dot single-photon turnstile device. Science 2000, 290: 2282–2285. 10.1126/science.290.5500.2282View Article
                5. Schneider C, Heindel T, Huggenberger A, Niederstrasser TA, Reitzenstein S, Forchel A, Höfling S, Kamp M: Microcavity enhanced single photon emission from an electrically driven site-controlled quantum dot. Appl Phys Lett 2012, 100: 091108–1–091108–4.View Article
                6. Salter CL, Stevenson RM, Farrer I, Nicoll CA, Ritchie DA, Shields AJ: An entangled-light-emitting diode. Nature 2010, 465: 594–597. 10.1038/nature09078View Article
                7. Mohan A, Felici M, Gallo P, Dwir B, Rudra A, Faist J, Kapon E: Polarization-entangled photons produced with high-symmetry site-controlled quantum dots. Nat Photonics 2010, 4: 302–306. 10.1038/nphoton.2010.2View Article
                8. Martín-Sánchez J, Muñoz-Matutano G, Herranz J, Canet-Ferrer J, Alén B, González Y, Alonso-González P, Fuster D, González L, Martínez-Pastor J, Briones F: Single photon emission from site-controlled InAs quantum dots grown on GaAs(001) patterned substrates. ACS Nano 2009, 3: 1513–1517. 10.1021/nn9001566View Article
                9. Felici M, Gallo P, Mohan A, Dwir B, Rudra A, Kapon E: Site-controlled InGaAs quantum dots with tunable emission energy. Small 2009, 5: 938–943. 10.1002/smll.200801274View Article
                10. Schneider C, Strauß M, Sünner T, Huggenberger A, Wiener D, Reitzenstein S, Kamp M, Höfling S, Forchel A: Lithographic alignment to site-controlled quantum dots for device integration. Appl Phys Lett 2008, 92: 183101–1–183101–3.
                11. Wang Zh M, Seydmohamadi Sh, Lee JH, Salamo GJ: Surface ordering of (In, Ga) As quantum dots controlled by GaAs substrate indexes. Appl Phys Lett 2004, 85: 5031–5033. 10.1063/1.1823590View Article
                12. Lee JH, Wang Zh M, Black WT, Kunets VP, Mazur YI, Salamo GJ: Spatially localized formation of InAs quantum dots on shallow patterns regardless of crystallographic directions. Adv Funct Mater 2007, 17: 3187–3193. 10.1002/adfm.200700066View Article
                13. Tommila J, Tukiainen A, Viheriälä J, Schramm A, Hakkarainen TV, Aho A, Stenberg P, Dumitrescu M, Guina M: Nanoimprint lithography patterned GaAs templates for site-controlled InAs quantum dots. J Cryst Growth 2011, 323: 183–186. 10.1016/j.jcrysgro.2010.11.165View Article
                14. Balzarotti A: The evolution of self-assembled InAs/GaAs(001) quantum dots grown by growth-interrupted molecular beam epitaxy. Nanotechnology 2008, 19: 505701. 10.1088/0957-4484/19/50/505701View Article
                15. Leon R, Fafard S: Structural and radiative evolution in quantum dots near the InxGa1-xAs/GaAs Stranski-Krastanow transformation. Phys Rev B 1998, 58: R1726-R1729. 10.1103/PhysRevB.58.R1726View Article
                16. Larsson LA, Larsson M, Moskalenko ES, Holtz PO: Temperature and magnetic field effects on the transport controlled charge state of a single quantum dot. Nanoscale Res Lett 2010, 5: 1150–1155. 10.1007/s11671-010-9618-xView Article
                17. Cho NK, Ryu SP, Song JD, Choi WJ, Lee JI, Jeon H: Comparison of structural and optical properties of InAs quantum dots grown by migration-enhanced molecular-beam epitaxy and conventional molecular-beam epitaxy. Appl Phys Lett 2006, 88: 133104–1–133104–3.
                18. O'Donnell KP, Chen X: Temperature dependence of semiconductor band gaps. Appl Phys Lett 1991, 58: 2924–2926. 10.1063/1.104723View Article
                19. Vurgaftman I, Meyer JR, Ram-Mohan LR: Band parameters for III–V compound semiconductors and their alloys. J Appl Phys 2001, 89: 5815–5875. 10.1063/1.1368156View Article
                20. Huang YS, Qiang H, Pollak FH, Pettit GD, Kirchner PD, Woodall JM, Stragier H, Sorensen LB: Temperature dependence of the photoreflectance of a strained layer (001) In0.21Ga0.79As/GaAs single quantum well. J Appl Phys 1991, 70: 7537–7542. 10.1063/1.349706View Article
                21. Ouerghui W, Melliti A, Maaref MA, Bloch J: Dependence on temperature of homogeneous broadening of InGaAs/InAs/GaAs quantum dot fundamental transitions. Physica E 2005, 28: 519–524. 10.1016/j.physe.2005.05.051View Article
                22. Cade NI, Gotoh H, Kamada H, Nakano H, Anantathanasarn S, Nötzel R: Optical characteristics of single InAs/InGaAsP/InP (100) quantum dots emitting at 1.55 μm. Appl Phys Lett 2006, 89: 181113–1–181113–3.View Article
                23. Selçuk E, Yu Silov A, Nötzel R: Single InAs quantum dot arrays and directed self-organization on patterned GaAs (311) B substrates. Appl Phys Lett 2009, 94: 263108–1–263108–3.View Article
                24. Tran T, Muller A, Shih CK, Wong PS, Balakrishnan G, Nuntawong N, Tatebayashi J, Huffaker DL: Single dot spectroscopy of site-controlled InAs quantum dots nucleated on GaAs nanopyramids. Appl Phys Lett 2007, 91: 133104–1–133104–3.View Article


                © Tommila et al.; licensee Springer. 2012

                This article is published under license to BioMed Central Ltd. This is an Open Access article distributed under the terms of the Creative Commons Attribution License (http://​creativecommons.​org/​licenses/​by/​2.​0), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.