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Planarization of InP pyramids containing integrated InAs

quantum dots and their optical properties

Citation for published version (APA):

Wang, H., Yuan, J., Veldhoven, van, P. J., Vries, de, T., Smalbrugge, E., Geluk, E. J., & Nötzel, R. (2010). Planarization of InP pyramids containing integrated InAs quantum dots and their optical properties. Journal of Applied Physics, 108(10), 104308-1/4. [104308]. https://doi.org/10.1063/1.3491025

DOI:

10.1063/1.3491025 Document status and date: Published: 01/01/2010

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Planarization of InP pyramids containing integrated InAs quantum dots

and their optical properties

Hao Wang,a兲Jiayue Yuan, René P. J. van Veldhoven, Tjibbe de Vries, Barry Smalbrugge, Erik Jan Geluk, and Richard Nötzel

Department of Applied Physics, COBRA Research Institute, Eindhoven University of Technology, 5600 MB Eindhoven, The Netherlands

共Received 24 June 2010; accepted 21 August 2010; published online 19 November 2010兲

Position-controlled InAs quantum dots共QDs兲 are integrated into planar InP structures by employing selective area growth of InP pyramids and regrowth by metalorganic vapor-phase epitaxy. A smooth surface morphology is obtained at elevated regrowth temperature due to suppression of three-dimensional growth on the pyramids. The height differences are less than 30 nm after nominal 700 nm InP regrowth at 640 ° C. Most important, the integrated QDs maintain good optical quality after regrowth for the realization of integrated nanophotonic devices and circuits operating at telecom wavelengths. © 2010 American Institute of Physics.关doi:10.1063/1.3491025兴

I. INTRODUCTION

Photonic integration shows a clear exponential increase in component density similar to Moore’s law in electronics.1 For further increase, in particular, quantum dot 共QD兲 gain material is appealing due to low transparency currents, very broad gain spectra, and the possibility of deep etching with-out device degradation. Extended cavity Fabry–Pérot QD la-sers have already been demonstrated based on established Butt-joint active-passive integration technology.2 Pushing photonic integration technology to the fundamental limits re-garding component size, complexity, and power consumption will require position control of QDs in small numbers, down to a single QD and novel integration techniques allowing device operation at the few/single electron and photon levels. Among the various approaches for QD position control based on growth on patterned substrates3–6and selective area growth7–13we have chosen the latter. The deposition of QDs on selectively grown pyramids allows not only QD position and number control but also the control of the QD distribu-tion through the pyramids base shape12 for matching it, e.g., to the optical mode of a particular photonic crystal nanocav-ity.

Here we demonstrate the integration of position con-trolled InAs QDs embedded in submicron-size InP pyramids into planar structures by regrowth of InP in metalorganic vapor-phase epitaxy 共MOVPE兲. Growth conditions are first optimized for nominal 250 nm InP regrowth and then trans-ferred to thicker layers for large-scale regrowth. A smooth surface morphology is obtained at elevated regrowth tem-perature due to suppression of three-dimensional growth on the pyramids. The height differences are less than 30 nm after optimized nominal 700 nm InP regrowth at 640 ° C and there is no growth on the pyramids top. Most important, good optical quality of the integrated QDs is maintained for the realization of integrated nanophotonic devices and cir-cuits operating at telecom wavelengths.

II. EXPERIMENTAL DETAILS

For substrate patterning a 100 nm SiNxmask layer was deposited on the InP 共100兲 substrates by plasma-enhanced chemical-vapor deposition. A field of openings in the mask was processed by electron beam lithography and reactive ion etching. The center-to-center distance of the openings was

a兲Electronic mail: wh-mouse@163.com.

(b) 2 × 2 μm2 [011] [01-1] [001] (a) 1 × 1 μm2 10× 10 μm2 (c) 4× 4 μm2 (d) 4× 4 μm2 (f) 4× 4 μm2 (e) 4× 4 μm2 (g) 4× 4 μm2 (h)

FIG. 1. 共Color online兲 AFM images of 共a兲 truncated pyramid with QD on top, 共b兲 CP, and 共c兲–共h兲 RPs with regrowth temperatures of 550 °C, 共e兲 585 ° C,共f兲 600 °C, 共g兲 615 °C, and 共h兲 630 °C. Diameter of the circular mask opening is 700 nm.

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10 ␮m. For selective area growth and regrowth, first, trun-cated InP pyramids were grown at 610 ° C by selective area MOVPE using tertiary butyl phosphine and trimethyl indium as precursors. Then the temperature was lowered to 500 ° C for growth of a GaAs interlayer共tertiary butyl arsine, trim-ethyl gallium兲, and the InAs QDs 共TBA, TMI兲. The GaAs interlayer tunes the QD emission wavelength into the 1.55 ␮m wavelength region.14After QD formation, an 8 nm InP capping layer was grown at 500 ° C, then the tempera-ture was raised to 610 ° C and another 40 nm InP cap layer was deposited. The detailed growth parameters can be found in Refs. 12and 13. The SiNx mask was then removed and

regrowth of 250 or 700 nm InP was performed at tempera-tures between 550 and 640 ° C. The surface morphology of the uncapped InAs QDs on the InP pyramids top, the fully capped pyramids 共CPs兲, and the regrown pyramids 共RPs兲 was examined by atomic force microscopy共AFM兲. The op-tical properties of the regrown InP and the capped and re-grown QDs were studied by microphotoluminescence 共micro-PL兲 spectroscopy with a spatial resolution of ⬃0.5 ␮m and the samples mounted in a He-flow cryostat. The PL was excited by the 632.8 nm line of a He–Ne laser through an optical microscope objective, which also served

to collect the PL. The PL was dispersed by a single mono-chromator and detected by a cooled InGaAs linear array de-tector.

III. RESULTS AND DISCUSSION

Figure 1 shows the AFM images of the uncapped InP pyramids and CPs before and after InP regrowth. The round shaped mask opening has a diameter of 700 nm. Figure1共a兲 reveals a single InAs QD on the InP pyramid close to pinch-off, Fig. 1共b兲 the CP after capping the QD, and Figs.

1共c兲–1共h兲the RPs after deposition of nominal 250 nm InP at the growth temperatures of 550 ° C, 585 ° C, 600 ° C, 615 ° C, and 630 ° C, respectively. Figure 2共a兲 depicts the corresponding line profiles taken along关011¯兴 and 关001兴, off-set by the thickness of the planar layers around the pyramids. The vertical solid black, dotted red, and dashed blue lines indicate the pyramids center, edge, and the planar areas. In Fig.2共b兲the regrown layer thicknesses at the pyramids cen-ter, edge, and of the planar layers aside are plotted as a function of regrowth temperature; in Fig.2共c兲the extension of the laterally grown layers around the pyramids along 关011¯兴 and 关001兴, and in Fig.2共d兲the angle of the sidewalls in

[01-1] 1.2 0.9 0.6 0.3 0.0 CP RP@550℃ RP@585℃ RP@600℃ RP@615℃ RP@630℃ (a) [001] 6 3 0 3 6 Distance (μm) H e ig ht (μm ) R egrowt h thi c k ness (μm ) Pyramid center Pyramid edge Planar area 1.0 0.8 0.6 0.4 0.2 0.0 500 550 600 650 Temperature (℃) (b) (c) [001] direction [01-1] direction 8 6 4 2 0 500 550 600 650 Temperature (℃) L atera l extens ion (μm ) (d) [01-1] direction [001] direction 50 40 30 20 10 0 500 550 600 650 Temperature (℃) S idewall a ngle (Degree)

FIG. 2.共Color online兲 共a兲 AFM line profiles taken along 关011¯兴 and 关001兴 of the CP and RPs for different regrowth temperatures, offset by the thickness of the planar layers around the pyramids. The vertical solid, dotted, and dashed lines indicate the pyramids center, edge, and the planar areas.共b兲–共d兲 Temperature dependence of the共b兲 regrown layer thickness at the pyramids center, edge, and of the planar layers aside, 共c兲 extension of the laterally grown layers around the pyramids along关011¯兴 and 关001兴, and 共d兲 angle of the sidewalls in the 关011¯兴 and 关001兴 directions between the laterally and planar grown layers.

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the关011¯兴 and 关001兴 directions between the laterally and pla-nar grown layers. Before regrowth, the height and diameter of the CP are 510 nm and 850 nm, respectively. After re-growth, with increasing temperature from 550 to 630 ° C: 共i兲 The regrown layer thickness at the pyramid center

reduces from 460 to 0 nm.

共ii兲 The layer thickness at the pyramid edge decreases from 930 to 260 nm.

共iii兲 The thickness of the planar layer around the pyramids increases from 0 to 230 nm, close to the thickness at the pyramid edge.

共iv兲 The extensions of the laterally grown layer around the pyramid along 关011¯兴 and 关001兴 reduce and become equal.

共v兲 The angles of the sidewalls in the 关011¯兴 and 关001兴 directions between the laterally and planar grown lay-ers reduce and become equal.

Therefore, with increase in the regrowth temperature there is a clear transition from three-dimensional asymmetric growth entirely on the pyramid to two-dimensional symmet-ric lateral and planar growth around the pyramid leading to planarization.

The growth rate enhancement at the pyramid edge is attributed to adatoms migrating from the pyramid side facets to the planar area and is reduced when planar growth domi-nates. The strong asymmetry of the three-dimensional growth at low temperature is due to the different growth rates on the pyramid facets. The growth rate on the共111兲B facets is the largest, leading to strong extension along关011¯兴, most probably due to its surface energy being the lowest.13 This growth asymmetry is also reflected in the different and rela-tively steep sidewall angles of the laterally grown layer around the pyramid. At high temperature, faceting becomes less pronounced and symmetric lateral and planar growth dominate, which is also seen in the almost identical and re-duced sidewall angles.

To perform larger-scale regrowth, the nominal InP layer thickness is increased to 700 nm and the growth temperature to 640 ° C. Figure 3 shows the AFM image of the regrown structure around a pyramid with base size of 1.5 ␮m to-gether with the line profile, including that of the CP. There is no growth on top of the pyramid. The growth rate

enhance-ment at the pyramid edge is reduced to 30 nm which is the same as the height difference of the laterally and planar grown layers. The extension of the laterally grown layer is increased to 5 ␮m with an overall very smooth surface mor-phology. The PL efficiency of the regrown InP is high, com-RP @ 640 ℃ CP 0 2 4 6 1.0 0.8 0.6 0.4 0.2 0.0 6 × 6 μm2 [011] [01-1] Distance (μm) Height (μm )

FIG. 3. 共Color online兲 AFM image of the optimized large-scale RP with base size of 1.5 ␮m together with the line profile, including that of the CP. Inserted arrow indicates the profile place and direction.

308 μeV 13.6 nW (P0) Energy (eV) (a) 5 K 0.840 0.845 0.850 0.855 50 40 30 20 10 0.0 PL intensit y (counts/sec ) 2.0 nm 0.5 nm 5 K (b) 104× P 0 102× P 0 10 × P0 P0 Wavelength (nm) 105 10 10 10 4 3 2 101 1 PL intensit y (counts/sec ) 1400 1425 1450 1475 1500 (c) 5 K 30 K 50 K 70 K 100 K 120 K Wavelength (nm) PL intensity (arb. units) 1400 1420 1440 1460 1480 1500 1.0 0.8 0.6 0.4 0.2 0.0 (d) 10 20 15 5 0 FWHM (nm ) 1490 1480 1470 1460 1450 0 30 60 90 120 150 PL peak position (nm ) Temperature (K)

FIG. 4. 共Color online兲 共a兲 Micro-PL spectrum of an integrated single QD after regrowth. 共b兲 Excitation power dependent micro-PL spectra. P0

= 13.6 nW. Resolution of monochromators is indicated. 共c兲 Temperature dependent micro-PL spectra and共d兲 plot of the QD PL peak position and FWHM vs temperature.

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parable to that of planar layers. This confirms good crystal quality and indicates a low level of nonradiative recombina-tion centers which is required for low absorprecombina-tion of the pas-sive structures in photonic integrated circuits.

Figure4 shows the micro-PL spectrum of an integrated single QD after regrowth taken at 5 K with 13.6 nW laser excitation power. The PL peak is centered at 0.8478 eV 共1462 nm兲 with a full-width at half maximum 共FWHM兲 of 308 ␮eV共0.5 nm兲. This is close to the resolution limit of our setup and most probably larger than the intrinsic linewidth due to pronounced broadening and redshift with excitation power already observed in this regime, as shown in Fig.4共b兲. When the excitation power is increased from 13.6 nW up to 136 ␮W the PL linewidth increases up to 6 nm and the PL peak shifts from 1462 to 1456 nm. This excitation power dependence is typical due to fluctuating charge distributions around the QD statistically shifting its energy levels, in par-ticular to lower energies due to the quantum confined Stark effect. Unfortunately the measurement sensitivity does not allow us to further reduce the excitation power below the 13.6 nW.

To definitely make sure that the emission stems from a single QD, temperature dependent PL spectra are taken, shown in Fig.4共c兲. The excitation power is 136 ␮W in order to trace the emission up to sufficiently high temperatures. With increasing temperature the PL peak redshifts from 1456 nm at 5 K to 1478 nm at 120 K, plotted in Fig.4共d兲, follow-ing the bandgap, typical for sfollow-ingle QDs. The FWHM does not change much below 50 K共from 6 to 7 nm兲, while there is a strong increase for higher temperatures. This again is typical for single QDs also on planar substrates due to the change over from acoustic to optical phonon scattering.15

IV. CONCLUSIONS

We have demonstrated the planarization of selectively grown submicron size InP pyramids containing integrated InAs QDs by regrowth of InP in MOVPE. Taking advantage of the two-dimensional lateral and planar growth around the pyramids at elevated growth temperatures, a smooth surface morphology is obtained. The height differences are less than

30 nm after optimized nominal 700 nm InP regrowth at 640 ° C and there is negligible growth on the pyramids. Most important, good optical quality of the integrated QDs is maintained after regrowth paving the way for the realization of integrated nanophotonic devices and circuits operating at telecom wavelengths.

ACKNOWLEDGMENTS

The authors gratefully acknowledge the support of ePIX-net 共EU兲 and the Smart Mix Programme of the Netherlands Ministry of Economic Affairs and the Netherlands Ministry of Education, Culture, and Science.

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