APL Photonics 3 , 116103 (2018); https://doi.org/10.1063/1.5050669 3 , 116103 © 2018 Author(s). Fabrication of dense diameter-tuned quantum dot micropillar arrays for applications in photonic information processing Cite as: APL Photonics 3 , 116103 (2018); https://doi.org/10.1063/1.5050669 Submitted: 02 August 2018 . Accepted: 12 September 2018 . Published Online: 28 September 2018 Tobias Heuser, Jan Große, Arsenty Kaganskiy, Daniel Brunner , and Stephan Reitzenstein ARTICLES YOU MAY BE INTERESTED IN Micropillars with a controlled number of site-controlled quantum dots Applied Physics Letters 112 , 071101 (2018); https://doi.org/10.1063/1.5017692 On-demand generation of background-free single photons from a solid-state source Applied Physics Letters 112 , 093106 (2018); https://doi.org/10.1063/1.5020038 Enhanced photon-extraction efficiency from InGaAs/GaAs quantum dots in deterministic photonic structures at 1.3 μm fabricated by in-situ electron-beam lithography AIP Advances 8 , 085205 (2018); https://doi.org/10.1063/1.5038137 APL PHO TONICS 3 , 116103 (2018) F abrication of dense diameter -tuned quantum do t micropillar array s for applications in pho tonic information processing T obias Heuser, 1 Jan Große, 1 Arsenty Kaganskiy, 1 Daniel Brunner, 2 and St ephan Reitzenstein 1, a 1 Institut f ¨ ur F estk ¨ orperphysik, T echnisc he Universit ¨ at Berlin, Har denber gstraße 36, D-10623 Berlin, Germany 2 FEMTO-ST/Optics Department, UMR CNRS 6174, Univversit ´ e Bour gogne F ranche-Comt ´ e, 15B A venue des Montboucons, 25030 Besanc ¸ on Cedex, F rance ( Receiv ed 2 August 2018; accepted 12 September 2018; published online 28 September 2018) W e report on the realization of a dense, large-scale array of 900 quantum dot micropil- lar ca vities with high spectral homogeneity . W e target applications in photonic infor - mation processing such as optical reserv oir computing which can be implemented in lar ge arrays of optically coupled microlasers. T o achiev e the required spectral homogeneity for the underlying optical injection locking, we calculate and set the diameter of each indi vidual micropillar within the array during the fabrication pro- cess by taking the diameter -dependent emission wav elength of the microcavities into account. Using this kind of diameter adjustment, we improv e the ov erall wa velength homogeneity in a 30 × 30 micropillar array by 64% and reduce the standard de vi- ation of the resonance ener gy distrib ution by 26% from 352 µ eV in the planar unprocessed sample to 262 µ eV in the f abricated array . In addition, we present a detailed analysis of the de vice quality and the diameter control of the micropillar’ s emission wa velength, which includes important information for the ef fecti ve applica- tion of the de veloped fabrication method for the realization of highly homogeneous micropillar arrays in the future. © 2018 A uthor(s). All article content, except wher e otherwise noted, is licensed under a Cr eative Commons Attrib ution (CC BY) license ( http://cr eativecommons.or g/licenses/by/4.0/ ). https://doi.or g/10.1063/1.5050669 I. INTRODUCTION The de velopment of high-quality quantum dot (QD) micropillar ca vities has enabled numerous studies and adv ances in the field of cavity-enhanced nanophotonic de vices. Besides the in v estigation of fundamental light-matter interaction in the single-QD regime of ca vity quantum electrodynamics (cQED), 1 , 2 appealing applications of QD-micropillars include single-photon sources with close to ideal optical properties 3 , 4 and high- β QD-microlasers 5 sho wing ev en single-QD lasing ef fects. 6 More recently , the study of externally controlled QD-microlasers has led to uncon v entional effects such as partial injection locking in the field of nonlinear laser dynamics. 7 , 8 Interestingly , so far the related research has almost exclusi v ely focused on indi vidual QD-microcavity systems without taking adv an- tage of coupling these de vices to larger systems with enhanced functionality . F or instance, network dynamics of coupled microlasers promise e xciting applications in adv anced photonic information pro- cessing such as neuromorphic computing. 9 , 10 These applications usually set stringent requirements on the fabrication of the microlasers since the y rely on an extremely well-defined separation (pitch) between the indi vidual lasers 10 and spectral homogeneity 11 within lar ge scale laser arrays, where pho- tonic neural networks typically require se veral hundred lasers 12 emitting within a frequenc y-range of ∼ 50 GHz ( ∼ 200 µ eV). a [email protected] 2378-0967/2018/3(11)/116103/9 3 , 116103-1 © Author(s) 2018 116103-2 Heuser et al. APL Photonics 3 , 116103 (2018) The realization of spectrally homogeneous microca vity arrays is not feasible by relying upon post-fabrication tuning methods commonly applied in single-QD e xperiments using temperature, 2 , 13 magnetic field, 14 , 15 or the electrical field. 16 , 17 This issue is e xplained by the fact that these param- eters mainly influence the emission ener gy of the excitonic emitters b ut hav e only minor ef fect, if any , on the spectral features of the cavity mode. Additionally , the tuning of individual pillars is not feasible in the case of global temperature or magnetic field tuning. T uning of indi vidual lasers via electrical contacts too is technologically very challenging and becomes increasingly dif ficult with increasing network size and density . Therefore, the spectral alignment of a lar ge-scale network of micropillars has to be ensured already in the ca vity design and fabrication process of the array , for example, by adjusting the resonance w av elength of each micropillar via its diameter . Interest- ingly , such “diameter -tuning” of the resonance wa velength has already been applied for indi vidual deterministically fabricated single-QD-micropillars. 4 , 18 In this w ork, we report on the application of diameter -tuning to realize lar ge arrays of hundreds of quantum dot micropillars with high spectral homogeneity . For this purpose, we indi vidually tailor the resonance wa velength of single micropil- lars to compensate for spectral inhomogeneities of the unprocessed planar microca vity . By applying this approach, we achie ve high spectral homogeneity of 262 µ eV within a lar ge-scale array of up to 900 quantum dot micropillars. Such homogeneity facilitates the interaction between the indi- vidual lasers of such arrays and allo ws them to form a network that can be optically injection- locked by using an e xternal laser . 11 II. METHOD AND SAMPLE TECHNOL OG Y The fabrication process for dense arrays of quantum dot micropillars starts with the epitax- ial gro wth of a planar microcavity sample by means of metal-or ganic chemical v apor deposition (MOCVD). The layer design of the planar microca vity consists of a central one- λ thick GaAs ca vity sandwiched between a lo wer and an upper distributed Bragg reflector (DBR) composed of 27 and 23 λ /4-thick Al 90 Ga 10 As/GaAs mirror pairs, respecti v ely . The central GaAs cavity includes a single layer of self-assembled Stranski-Krastano w InGaAs QDs with a density of about 1 × 10 10 cm − 2 . During the gro wth process, the material deposition depends on the radial position of the rotating wafer which causes a radial layer thickness v ariation of about 2% (3 nm per DBR pair) and, in return, leads to an associated radial dependence of the ca vity resonance wav elength. This typical and gen- erally una voidable radial v ariation of the resonance wa velength in the epitaxial microca vity growth is illustrated in Fig. 1(a) , which sho ws the resonance wa velength of the planar microca vity from the center to the edge of a 2 inch wafer . For the particular sample of Fig. 1 , the ca vity exhibits a total radial shift of its resonance by about 25 nm. T o realize homogeneous arrays of micropillar lasers, part of this resonance shift has to be compensated by adjusting the pillar diameters within the 300 × 300 µ m 2 sample area rele vant for the 30 × 30 micropillar array with a pitch of 10 µ m chosen in this w ork. For this purpose, we consider the well-kno wn relation between the micropillar diameter d c and the resonance ener gy E c of the pillar modes, 19 , 20 E c = s E 2 0 + α r ~ 2 c 2 ε r 4 x 2 ϕ , r d 2 c , (1) where E 0 is the position dependent resonance energy of the planar microca vity , ε r is the effecti ve dielectric constant of the ca vity material, and x ϕ , r is the n th r zero of the Bessel function J ϕ ( x ), which has a numeric v alue of 2.4048 for the fundamental HE 11 mode. W e introduced the additional parameter α r which takes the process dependent light confinement into account. It is interesting to note that there exists a trade-of f between the achie v able spectral compensation and the variations in the pillar emission ener gy induced by a gi ven diameter accurac y . The E c ( d c ) becomes steeper with decreasing diameter allo wing for a larger spectral compensation. Consequently , E c becomes more sensitiv e to small v ariations in d c which can lead to process related spectral inhomogeneities. On the other side, this beha vior allows to adjust the tuning windo w of this method to a gi ven process accurac y . In practice, we can achie ve a spectral compensation of about 5–8 meV in the rele v ant diameter range of 2–6 µ m. 116103-3 Heuser et al. APL Photonics 3 , 116103 (2018) FIG. 1. (a) One dimensional µ PL scan of the resonance wav elength along the radius of an unprocessed 2 in. wafer . The scan indicates a gro wth related radial shift of the unprocessed wafer’ s resonance wa velength by about 25 nm. In our nanofabrication process, this shift is compensated by precisely setting the radius of each indi vidual QD-micropillar within a dense array during electron-beam lithography (EBL). Inset: Emission spectrum at a radial position of 9.7 mm from the edge of the wafer . [(b)–(e)] Scanning electron microscopy (SEM) images of the fabricated hard-masks and micropillar arrays with 900 resonators with a spatial pitch of about 10 µ m. T o calculate the required diameter for each micropillar in the 30 × 30 array , first α r has to be determined for the chosen etching process as we describe belo w . Then the resonance energy of the desired sample area needs to be mapped by micro-photoluminescence ( µ PL) map-scans cov ering the rele vant area of about 300 µ m × 300 µ m. Here, the pitch between each pixel of the map- scans corresponds to the pitch (10 µ m) of the final micropillar array so that each scanned pixel is associated with an indi vidual pillar in the final array . T o facilitate the calculation of the pillar diameters according to Eq. ( 1 ) with respect to a chosen tar get emission energy E c , the measured wa velength data from the map-scans are first fitted by a polynomial function of 5th-order . The resulting calculated laser diameter pattern for the 30 × 30 pillar array is then transferred to the sample via electron- beam lithography (EBL) by using a scanning electron microscope equipped with a pattern generator . The process starts with coating of the sample with a SiN layer using plasma enhanced chemical v apor deposition (PECVD). This layer acts as material for a hard mask which ensures a high etch selecti vity for the following plasma etching steps. Then the sample is coated with a ne gati ve-tone EBL-resist which is exposed using the calculated pattern of the pillar array that can be aligned with an accuracy of about 5 µ m to the desired sample area. Afterw ard, the pattern is transferred into the 500 nm thick SiN layer by a reacti ve ion etching (RIE) process using a SF 6 plasma. This results in a hard mask with smooth vertical side walls, as illustrated in Fig. 1(b) . Finally , the pillar structures 116103-4 Heuser et al. APL Photonics 3 , 116103 (2018) [Figs. 1(c) – 1(e) ] are etched by an inducti vely coupled plasma (ICP) RIE process using a mix ed plasma recipe containing Ar 2 , Cl 2 , and BCl 3 . The etching process by which we remov e the upper DBR and up to 20 mirror pairs of the lo wer DBR is optimized to achiev e vertical side-w alls. W e would like to note that process imperfections lead to (unintentional) statistical v ariations in the pillar diameters with a standard de viation of approximately 30 nm. III. EXPERIMENT AL SETUP AND OPTIC AL CHARA CTERIZA TION Optical characterization is performed by means of high resolution µ PL spectroscop y . The sample is placed onto a motorized x-y-z stage with sub- µ m accurac y in all three dimensions. All measure- ments are performed at room temperature. Optical e xcitation is realized by using a diode pumped solid-state laser emitting at 671 nm which is focused via a microscope-objecti ve (N A = 0.4) onto the surface of the sample. An additional x-y-z piezo-stage ensures spatial fine adjustment of the micro- scope objecti ve. The µ PL signal of the micropillar structures is then collected by using the same microscope objecti ve and detected via a grating spectrometer with a spectral resolution of about 20 µ eV , where a pinhole is used in a confocal microscope to selecti vely collect µ PL signal from indi vidual micropillars. The setup is automatized to record the PL emission from each individual micropillar in the 30 × 30 array . Here, the x-y-z piezo-stage is used for additional precise auto- adjustment for each indi vidual micropillar in the array via an optical feedback-loop. This way , a spectral map is recorded in which each pix el is associated with the spectral information of a single micropillar inside the array . W e first ev aluate the quality of the de vice fabrication by a diameter dependent optical character - ization of a series of reference micropillars processed by the nominally same method as used for the micropillar arrays to be discussed belo w . The results are illustrated in Fig. 2 , which shows a typical emission µ PL spectrum (a) of a 4 µ m micropillar , as well as the ca vity Q-factor (b) and the funda- mental resonance ener gy E c (c) vs pillar diameter d c . The 4 µ m micropillar ca vity sho ws a distinct mode spectrum with fundamental HE 11 mode at 1.1625 eV (1066.51 nm) and a Q factor of 5450. The emission wa velength of about 1060 nm w as chosen in our work to match the requirements of an existing setup for the implementation of optical reserv oir computing. The diameter dependent data presented in the lo wer panels show the typical decrease in the Q-f actors with decreasing diameter due to enhanced losses in the small diameter regime. 21 Additionally , when compared to theoretical v alues of about 16 000 obtained by using finite-element simulations, 22 experimental Q-factors up to 6000 at lar ge diameters indicate absorption losses in non-ideal DBR sections and in the acti ve area. 21 The experimental E c ( d c ) dependence sho ws a pronounced diameter dependent blue-shift and is quantitati vely described by Eq. ( 1 ). The fit yields E 0 = 1.160 840 eV ± 22 µ eV and α r = 0.95 ± 0.01 which were used to calculate the diameter for each micropillar in the homogeneous array according to Eq. ( 1 ). It is important to note that successful diameter tuning depends sensiti vely on the precise kno wledge of the process related parameter α r which influences the slope of the E c ( d c ) dependence in particular at lo w diameters. Here, α r is a measure of the lateral light-confinement capabilities of the micropillars and increases with improv ed lateral light confinement. T o obtain better insight into this important parameter , we numerically simulated the diameter dependent mode properties of micropillar ca vities under v ariation of the etching depth for two dif ferent DBR compositions and slightly dif ferent resonance wa velengths using a commercial finite-element-method solv er . 22 Fitting the calculated E c ( d c ) dependencies allo ws us to determine the associated α r parameters [see Eq. ( 1 )] which are plotted in Fig. 2(d) vs the number of etched mirror pairs in the lo wer DBR for two dif- ferent material compositions. As expected, α r increases with the number of etched bottom DBR pairs because of higher lateral light confinement. On the other hand, α r is nearly independent of the resonance wa velength and the inde x contrast in the DBR, which increases slightly by changing the Al content from 90% to 100% due to enhanced vertical light confinement. This result highlights that α r is mainly influenced by the process related lateral mode confinement. For more than 10 etched mirror pairs in the lo wer DBR, the lateral light confinement becomes independent of the etching depth and α r saturates. This is the regime which we use in our w ork. Next we study the ef fect of diameter tuning on the spectral homogeneity of a processed 30 × 30 micropillar array . Figures 3 and 4 present spectroscopic results obtained for such a 116103-5 Heuser et al. APL Photonics 3 , 116103 (2018) FIG. 2. (a) µ PL emission spectrum of a micropillar with a diameter of 4 µ m, (b) cavity Q-Factor and line width, and (c) resonance energy as a function of the pillar diameter . (d) Simulations of the process parameter α r as a function of the etching depth for two dif ferent compositions (Al 90 Ga 10 As/GaAs and AlAs/GaAs) of the DBR sections and different resonance wa velengths (1050, 1060, and 1070 nm). The dependence re veals that the light confinement is reduced for lo w etching depths and remains almost constant for more than 10 etched bottom DBR mirror pairs, which is the regime in which we are working. 116103-6 Heuser et al. APL Photonics 3 , 116103 (2018) FIG. 3. µ PL map-scan of the resonance wa velength of the unprocessed sample region (a) and the map of the calculated diameters for 30 × 30 micropillar array (b) based on the fit of the resonance wa velength sho wn in Fig. 4(a) . (c) µ PL map-scan of the HE11 resonance wa velength of the fabricated array . As the color scale shows, the w av elength trend of the unprocessed material gets compensated by the ef fect of the diameter tuning. micropillar array . The array was f abricated in a sample region, marked in Fig. 1(a) , with a significant radial dependence of 2.1 nm/mm of the planar ca vity resonance to demonstrate the proposed concept of diameter tuning. This spectral trend is also seen in the resonance map-scan of the unprocessed material in Fig. 3(a) , where the resonance wa velength decreases from the top right to the bottom left corner of the map from 1058.33 nm to 1055.84 nm. This change in the resonance is accompanied by additional gro wth-related local resonance fluctuations throughout the sample region resulting in 116103-7 Heuser et al. APL Photonics 3 , 116103 (2018) FIG. 4. (a) 2D surface plots corresponding to a polynomial fit to the µ PL map-scans of the resonance wav elengths presented in Fig. 3 . The plot of the unprocessed sample region has a maximum resonance w avelength dif ference of 0.706 nm which is reduced to 0.254 nm in the micropillar array after applying diameter tuning. (b) Histogram of the resonance wa velengths of the planar microresonator and of micropillars in the fabricated array . (c) Slope dE c / dd c as a function of the pillar diameter plotted for the processing parameters presented in this letter . The curv e is showing the increasing influence of EBL accurac y with decreasing pillar diameter . an a verage resonance wa velength of 1057.49 nm and a standard de viation of 0.32 nm (352 µ eV). The diameters needed to compensate the radial resonance shift, sho wn in Fig. 3(b) , were calculated from the polynomial fit of this spectral map which is presented in the upper panel of Fig. 4(a) . 116103-8 Heuser et al. APL Photonics 3 , 116103 (2018) The fit also sho ws a maximum wav elength dif ference of about 0.71 nm across the chosen 300 × 300 µ m 2 sample area. This w av elength dif ference is smaller than the difference of the e xtreme v alues mentioned abov e because the fit leads effecti vely to an a veraging of the w av elengths. In our process, the spectral inhomogeneity of the planar microca vity is compensated by a diameter variation in the range from 3656 nm to 4240 nm. Here, the large diameter re gime was used to ensure that the tar get resonance wa velengths of the pillars are rather insensiti ve ag ainst process related diameter v ariations. The effecti v eness of the diameter tuning is clearly visible in Fig. 3(c) which presents a 2D map of the fundamental (HE 11 ) mode’ s resonance w a velength of the fabricated array . The color scale, which cov ers the same wa velength range of 2.49 nm for both maps, sho ws that the resonance wa velength gradient is clearly reduced on the fabricated micropillar array . A quantitativ e comparison between the planar sample before processing (fitted data) and the fabricated micropillar array sho ws that the maximum resonance wa velength dif ference could be decreased from 0.71 nm to 0.25 nm, which means a relati ve reduction by 64%; see Fig. 4(a) . Similarly , the standard de viation of the res- onance wa velength is reduced from 0.32 nm (352 µ eV) to 0.23 nm (262 µ eV), which can be seen in the statistical analysis of both µ PL map-scans in Fig. 4(b) . As expected from the Q-f actor vs diameter dependence presented in Fig. 2(a) , the diameter tuning also impacts the Q-factor within the array and can become quite significant in the small diameter range. In the present case, this side ef fect leads to a modest Q-factor dif ference of about 6% between the smallest and lar gest micropillars in the array and is not critical for the desired application in optical reserv oir computing. W e would like to note that despite the ov erall improv ement of the spectral homogeneity , local fluctuations up to 0.21 nm (230 µ eV) appear in the compensated array . This value w as determined by the av erage resonance dif- ference between a pillar and its four nearest neighbors. The reason for this shortcoming is the fact that local resonance v ariations of the planar microcavity are mask ed by the (global) polynomial fit of the planar ca vity’ s resonance wa velength. In future e xperiments, we plan to reduce the local variations by an optimized defect free epitaxial gro wth process and by calculating the micropillar diameter based directly on the local resonance wa velength without polynomial fitting. The latter requires a precise alignment of the processed pillar array with the scanned micropillar area by using suitable marker structures. By a suitable optimization of the reactor and the epitaxial gro wth process, it might become possible to almost completely suppress the radial dependence of the resonance wa velength already during sample gro wth. Even in this ideal case, our diameter -tuning scheme would be very beneficial to tailor the emission wa velength of the microca vities to meet the specific needs of the gi ven appli- cations. Considering also local v ariations in the resonance wa velength in the pillar -tuning process, the achie vable spectral homogeneity is mainly limited by the accuracy of the EBL system used in the fabrication process. T o determine the ef fect of diameter de viations from the calculated pattern, we calculated the slope dE c / dd c of the HE11 mode ener gy for parameters of the presented sample, which is sho wn in Fig. 4(c) . The plot rev eals that dE c / dd c changes in the used diameter windo w for this sample in a range between 1.01 and 1.59 µ eV/nm. Gi ven the mentioned writing error of our EBL system of up to 30 nm, this would lead to an achie v able spectral homogeneity as low as 0.054 nm (59 µ eV) for the gi ven sample parameters, which is around a f actor of 4.4 lower than the presently achie ved v alue of 0.23 nm (262 µ eV). Considering a diameter accurac y of 10 nm achie vable in state-of-the-art EBL systems, 23 the spectral homogeneity could be enhanced by an additional factor of about three when using such technology in the future. In this case, it could become important to consider and compensate also the typical fundamental mode splitting on the order of a fe w 10 s of µ eV which is related to a usually unintentional asymmetry of the pillar’ s cross section. 21 Finally , we would lik e to point o ut that for the application of diameter tuning, of course the spectral gradient of the wafer material which has to be compensated and the need for similar dynamical and optical properties of the indi vidual cavities ha ve to be considered because both factors limit the choice of a vailable diameter tuning-windo w and with this the achie vable compensation. IV . SUMMAR Y AND CON CL USION In summary , we proposed and demonstrated diameter tuning as an attracti ve method to impro ve the spectral homogeneity of lar ge scale micropillar arrays. As a spectral tuning method, we use the diameter dependence of the micropillar emission ener gy , which increases with decreasing pillar size 116103-9 Heuser et al. APL Photonics 3 , 116103 (2018) due to enhanced optical-mode confinement. W e realized a 30 × 30 array of micropillars and present experimental results which sho w that the maximum resonance wa velength dif ference could be reduced via diameter tuning by 64% from 0.71 nm to 0.25 nm if compared to v alues of the unprocessed planar wafer material. Related to that, a high homogeneity in terms of the standard de viation of the fundamental mode’ s emission wav elength of 262 µ eV (0.23 nm) w as achie ved. Ev en higher spectral homogeneity should be achie vable in the future by considering not only large scale v ariations b ut also local fluctuations in the resonance wa velength of the wafer material when determining the pillar diameters for compensation. Overall, the diameter tuning method has sho wn promising possibilities for the realization of homogeneous, lar ge-scale microlaser systems, for instance, for applications in optical neuromorphic computing. A CKNOWLEDGMENTS The research leading to these results recei ved funding from the V olkswagen F oundation via Neu- roQNet, the European Research Council under the European Union’ s Sev enth Frame work Program Grant Agreement No. 615613, and the German Research Foundation via No. CRC 787. 1 J. G ´ erard, B. Sermage, B. Gayral, B. Legrand, E. Costard, and V . Thierry-Mieg, Phys. Re v . Lett. 81 , 1110 (1998). 2 J. P . Reithmaier, G. Sek, A. L ¨ of fler, C. Hofmann, S. Kuhn, S. Reitzenstein, L. V . Keldysh, V . D. Kulako vskii, T . L. 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