We present the fabrication of strain-free quantum dots in the In0.53Ga0.47As/In0.52Al0.48As-system lattice matched to InP, as future sources for single and entangled photons for long-haul fiber-based quantum communication in the optical C-band. We achieved these quantum dots by local droplet etching via InAl droplets in an In0.52Al0.48As layer and subsequent filling of the holes with In0.53Ga0.47As. Here, we present detailed investigations of the hole morphologies measured by atomic force microscopy. Statistical analysis of a set of nanoholes reveals a high degree of symmetry for nearly half of them when etched at optimized temperatures. Overgrowth with 50–150 nm In0.52Al0.48As increases their diameter and elongates the holes along the [01]-direction. By systematically scanning the parameter space, we were able to fill the holes with In0.53Ga0.47As, and by capping the filled holes and performing photoluminescence measurements, we observe photoluminescence emission in the O-band up into the C-band depending on the filling height of the nanoholes.
I. INTRODUCTION
Many quantum communication protocols require sources capable of generating on-demand entangled photon pairs. For long-haul communication, these photons are generated ideally in the optical C-band (1530–1565 nm), where transmission losses inside silica fibers are minimal. Epitaxially grown semiconductor quantum dots (QDs) have been identified as very promising sources for single photons and entangled photon pairs.1,2 Most work has been done here in the near-infrared spectral range (around 930 nm) employing InAs QDs in a GaAs matrix and it has been shown that entangled photon pairs can be generated from the biexciton–exciton cascade of a single QD.3 Recently, entangled photon pairs have also been demonstrated in the optical C-band employing InAs QDs in an InxGa1−xAs matrix fabricated via the strain-driven Stranski–Krastanov (SK) growth mode4,5 and also by droplet epitaxy grown InAs QDs embedded in InP.6
However, despite all advantages as high emission rate and compatibility with mature semiconductor heterostructure technology, when QDs are used for the generation of entangled photon pairs, these bring their own set of challenges. The most important is that a reduction in symmetry results in an energetic splitting of the exciton level, called fine structure splitting (FSS), due to asymmetric wave functions. Because of the FSS, the exciton state is precessing, resulting in a time dependent entangled state.7,8 The reason for the reduction in symmetry is manifold: anisotropy of strain, shape, and composition. All these are related to the fabrication process and are quite pronounced in the usually employed strain-driven SK growth mode, especially the unavoidable anisotropic strain.9
One possible solution to reduce the FSS is not to rely on strain-driven epitaxy but to employ a different fabrication route resulting in unstrained QDs: filling of nanoholes fabricated via local droplet etching (LDE).10–12 Here, group III material, e.g., Al, is deposited without As flux on a III-V semiconductor layer (e.g., AlxGa1−xAs). This results in metallic droplet formation in a Volmer–Weber growth mode. In a subsequent annealing step, As from the semiconductor layer diffuses into the droplet due to the concentration gradient, which liquefies the region below the droplet. Finally, this results in a nanohole and a surrounding ring structure.13,14 These nanoholes are filled in a last step by a semiconductor with a lower bandgap (e.g., GaAs) and subsequent overgrowth with barrier material (e.g., AlxGa1−xAs).2,15,16 In the GaAs/AlAs system, this is a well-established process, and high-symmetry QDs with very low FSS have been produced.17–22 These QDs have been used, for example, to produce entangled photon pairs with very high fidelity2,23–25 and to generate photons that can be interfaced with Rb vapor as quantum memory.22,26
It is a straightforward idea to translate this concept to InxGa1−xAs QDs in an InxAlyGa1−x−yAs matrix, both approximately lattice matched to InP substrates, to achieve photon emission in the optical C-band. Here, nanoholes are etched into an InxAlyGa1−x−yAs layer lattice matched to InP and these holes are filled with In0.53Ga0.47As to obtain strain-free QDs. However, additional challenges arise due to the fact that now ternary or even quaternary alloys are involved: one has to hit the right composition to be fully lattice-matched and to create no defects. Also, it is questionable, if the composition of the ternary/quaternary alloys is maintained during hole etching, ring formation, and hole filling, respectively. So far, progress in this field has been elusive. Recently, first success in generating holes in In0.55Al0.45As on InP has been reported;27 however, as for now, there have been no reports of nanohole filling or optical emission in the C-band from strain-free QDs generated by filling of nanoholes on layers lattice-matched to InP.
In this paper, we report on the first successful filling of holes etched into In0.52Al0.48As layers with In0.53Ga0.47As, i.e., lattice-matched to InP. We analyzed in detail the morphological properties of the nanoholes generated at different temperatures between 390 and 505 °C. Furthermore, we have studied the overgrowth of nanoholes with In0.52Al0.48As and found that we were able to modify their in-plane symmetry and the size of the surrounding ring structure. We also demonstrate the filling of holes with different amounts of In0.53Ga0.47As and overgrowth of filled holes with a capping layer. For these structures, we present macro photoluminescence measurements and as well demonstrate single dot emission. We observed, depending on the filling level of the nanoholes, emission from the O-band up into the C-band.
II. EXPERIMENTAL DETAILS
All samples were grown on semi-insulating InP(100) substrates in a solid source molecular beam epitaxy (MBE) system equipped with an As cracker cell but no phosphorous source. The substrate temperature was measured by band-edge thermometry employing a BandiT system from KSA.28,29 Before the growth starts, all InP substrates were de-oxidized at 540 °C for 10 min under an As2 beam equivalent pressure (BEP) of pAs2 = 2.0 × 10−5 mbar. After de-oxidation, 100 nm lattice-matched In0.52Al0.48As was grown at 505 °C employing also an As2 pressure of pAs2 = 2.0 × 10−5 mbar. These parameters resulted in very smooth surfaces with a root-mean-square (rms) usually below 0.4 nm determined from atomic force microscope (AFM) images of the surface.
After the deposition of the initial In0.52Al0.48As layer, the substrate temperature was lowered at a nominal rate of 15 K min−1 for the droplet etching step. After reaching the target temperature Tetch ranging from 390 to 505 °C, the As flux was stopped, and after a break of 30 s, the In and Al shutters were opened simultaneously for 6 s. The In0.52Al0.48 amount deposited corresponds to a homogeneous In0.52Al0.48As thickness of 4.1 Ml, and the residual As pressure was approximately pAs2 = 1.8 × 10−6 mbar, i.e., roughly 1/10 of the As2-pressure used for the growth of the other layers. After the droplet deposition, an annealing step at the deposition temperature of 3 min was employed for the etching. A 6 min annealing step was also tested but it showed very similar results for the hole morphology; hence, we present here only results for the 3 min annealing step. After the annealing, the As flux was resumed and the holes were either overgrown by 50–150 nm In0.52Al0.48As while preserving the nanoholes or the holes were directly filled. For the overgrowth of the nanoholes, the substrate temperature was raised to 505 °C under an As2 pressure of pAs2 = 2.0 × 10−5 mbar.
Filling of the nanoholes was performed by depositing In0.53Ga0.47As at 505 °C with a very low average growth rate of roughly 0.7 Ml/min. This was achieved by depositing In0.53Ga0.47As cyclically, with 1 s of deposition corresponding to 0.7 Ml and 1 min growth interruption. This method was employed to enable a high surface diffusion time to allow the adatoms to migrate into the nanoholes. The filling of nanoholes was performed either under As2 or As4 atmosphere. For optical investigations, a capping layer of 100 nm In0.52Al0.48As was grown on top of the filled holes followed by a thin layer (5–10 nm) of In0.53Ga0.47As to protect the In0.52Al0.48As from oxidation.
To investigate the surface morphology at certain points in the process, growth was terminated after the relevant step, e.g., the etching step, the overgrowth of the nanoholes, or the filling of the nanoholes. The temperature was quenched at a rate of 25 K min−1 to 250 °C and the sample was taken out of the MBE system and investigated by AFM in the contact mode or by scanning electron microscopy. The samples with filled and capped nanoholes were investigated by standard photoluminescence spectroscopy at low temperatures (∼16 K) employing the above bandgap excitation at 532 nm.
III. NANOHOLE MORPHOLOGY
To better understand the shape of the nanoholes formed at the different temperatures, we individually analyzed more than 200 of them by AFM and summarized the average results for the geometry in Table I for Tetch = 390, 410, 435, and 460 °C and different overgrowth thicknesses dovergrowth. It was found that the general shape of the holes can be conserved when overgrowing them with In0.52Al0.48As at Tovergrowth = 505 °C under As2 environment. For Tetch = 480 and 505 °C, nearly all measurements showed the formation of two or three highly elongated holes inside of a single ring structure so no data for these etching temperatures are included in Table I. Parameters of the nanoholes were determined by evaluating AFM profiles in the [011]- and [01]-directions as indicated in Fig. 2.
Tetch . | 390 °C . | 410 °C . | 435 °C . | 460 °C . | ||||||
---|---|---|---|---|---|---|---|---|---|---|
dovergrowth | 0 nma | 0 nmb | 50 nmb | 100 nma | 150 nma | 0 nmb | 50 nmb | 150 nma | 0 nmb | 50 nmb |
h (nm) | 7.4 ± 1.1 | 18.9 ± 3.0 | 17.5 ± 2.7 | 16.8 ± 2.2 | 14.6 ± 1.9 | 22.9 ± 2.1 | 25.2 ± 2.3 | 17.6 ± 3.4 | 30.7 ± 3.8 | 33.1 ± 4.5 |
r (nm)c | 5.3 ± 0.6 | 13.1 ± 1.3 | 5.0 ± 0.8 | 1.6 ± 0.5 | 0.2 ± 0.3 | 12.7 ± 1.0 | 7.2 ± 0.6 | 0.7 ± 0.4 | 16.5 ± 2.1 | 11.0 ± 1.6 |
d[011] (nm) | 90 ± 14 | 138 ± 13 | 137 ± 29 | 170 ± 22 | 185 ± 25 | 183 ± 26 | 193 ± 31 | 208 ± 34 | 272 ± 36 | 276 ± 23 |
(nm) | 101 ± 16 | 143 ± 13 | 149 ± 14 | 225 ± 14 | 352 ± 42 | 167 ± 19 | 183 ± 23 | 299 ± 78 | 197 ± 41 | 226 ± 44 |
Elongationd | 0.91 | 0.94 | 0.93 | 0.75 | 0.54 | 1.08 | 1.05 | 0.74 | 1.35 | 1.25 |
% sym. holese | 10 | 12 | 32 | 0 | 0 | 12 | 44 | 0 | 0 | 5 |
Tetch . | 390 °C . | 410 °C . | 435 °C . | 460 °C . | ||||||
---|---|---|---|---|---|---|---|---|---|---|
dovergrowth | 0 nma | 0 nmb | 50 nmb | 100 nma | 150 nma | 0 nmb | 50 nmb | 150 nma | 0 nmb | 50 nmb |
h (nm) | 7.4 ± 1.1 | 18.9 ± 3.0 | 17.5 ± 2.7 | 16.8 ± 2.2 | 14.6 ± 1.9 | 22.9 ± 2.1 | 25.2 ± 2.3 | 17.6 ± 3.4 | 30.7 ± 3.8 | 33.1 ± 4.5 |
r (nm)c | 5.3 ± 0.6 | 13.1 ± 1.3 | 5.0 ± 0.8 | 1.6 ± 0.5 | 0.2 ± 0.3 | 12.7 ± 1.0 | 7.2 ± 0.6 | 0.7 ± 0.4 | 16.5 ± 2.1 | 11.0 ± 1.6 |
d[011] (nm) | 90 ± 14 | 138 ± 13 | 137 ± 29 | 170 ± 22 | 185 ± 25 | 183 ± 26 | 193 ± 31 | 208 ± 34 | 272 ± 36 | 276 ± 23 |
(nm) | 101 ± 16 | 143 ± 13 | 149 ± 14 | 225 ± 14 | 352 ± 42 | 167 ± 19 | 183 ± 23 | 299 ± 78 | 197 ± 41 | 226 ± 44 |
Elongationd | 0.91 | 0.94 | 0.93 | 0.75 | 0.54 | 1.08 | 1.05 | 0.74 | 1.35 | 1.25 |
% sym. holese | 10 | 12 | 32 | 0 | 0 | 12 | 44 | 0 | 0 | 5 |
Sample size of 10.
Sample size of 25.
First averaged for every ring by measuring scan lines at 45° steps, then averaged across every set of measured rings.
Averaged value for the hole elongation. Elongation for a hole was calculated by dividing d in [011] by d in [01]. Values larger than 1 indicate a general elongation in [011], and values smaller than 1 in [01].
Fraction of symmetric holes in percent. A hole is classified as symmetric if all of the following criteria are fulfilled: (1) The ratio of diameters in [011]- and [01]-directions is close to 1. (2) For each direction, the ratio of the diameter and the distance s from the lowest point of the hole to the ring is close to 2. (3) No other obvious symmetry breaks are present.
As the symmetry of the nanoholes is a very important aspect of their application as QD photon sources, we tried to quantify this aspect for the nanoholes produced at the various parameters that we tested. For this, we chose three different requirements that an individual hole had to satisfy to be classified as symmetric: First, the ratio of diameters in [011]- and [01]-directions, which would be 1 for an ideal circular hole. Deviation from this value suggests elongation of the hole in either the [011]- (ratio > 1) or the [01]-direction (ratio < 1). Second, for each of the two crystalline directions, the ratio of the diameter d and the length s from the lowest point of the hole to the ring quantifies the level of skewness of a hole and would ideally be 2 for a perfect hole, where the deepest point is right in the center of the hole. An example for the failure of this criterion can be seen with the nanohole in Fig. 2(e), where the deepest point is shifted to the right. For these first two conditions, we chose a tolerance of 10% from their ideal values else a measured nanohole would be classified as asymmetric. The last requirement is that no other obvious symmetry breaks can be identified during measurement. Ideally, the nanoholes possess a cone-like profile, as can be seen exemplary in Fig. 2(d). Deviations from this shape, e.g., plateaus or double holes, would also result in a classification as asymmetric even if criteria 1 and 2 are fulfilled.
As listed in Table I, the depth for the non-overgrown nanoholes increases significantly from ∼7 nm at Tetch = 390 °C to ∼30 nm at Tetch = 460 °C. Thus, the volume of the hole (as well as the volume of the ring) increases with increasing Tetch. The volume increase is a result of the larger droplets generated at elevated temperatures. Higher temperature during droplet deposition improves the adatom surface diffusion and enables the formation of fewer, but larger droplets, resulting in an increased number of metal atoms contributing to the etching process generating deeper and wider holes and larger rings.
This effect results in larger diameters d of the nanoholes, as well. The average value for d increases from ∼100 nm for Tetch = 390 °C to above 200 nm at Tetch = 460 °C for non-overgrown nanoholes. However, we observe that, for increasing etching temperatures, our nanoholes develop a preferred elongation in the [011]-direction. This can be clearly seen at Tetch = 460 °C where the average d in [011] is much larger than in [01]. At this etching temperature, all measured nanoholes showed a preferred elongation in this direction. At the lower etching temperatures, e.g., at Tetch = 390 °C, we observe the opposite. Here, we find that a large fraction of the nanoholes is elongated in [01]-direction, but not all. A few of the measured nanoholes showed a slight elongation in the [011]-direction. We observe that by raising Tetch, the ratio of nanoholes elongated in [011] increases until Tetch ≥ 460 °C where all measured non-overgrown nanoholes were elongated in [011].
Due to this preferred elongation, we observe, for Tetch ≥ 435 °C, a very low fraction of non-overgrown nanoholes that fulfill our first criterion for symmetry (d ratio close to 1), resulting in only 12% symmetric nanoholes for Tetch = 435 °C and none for even higher temperatures. For non-overgrown samples produced at Tetch = 390 °C and Tetch = 410 °C, the fraction of nanoholes generated with good diameter ratios was much better, with more than 50%, which would suggest that these temperatures are ideal for generating symmetric nanoholes. However, here, most of the nanoholes also exhibited an incomplete hole formation, deviating from the ideal cone-like shape shown in Figs. 2(b) and 2(d). Because such a large amount of the measured nanoholes failed our third symmetry criterium, we find only a low fraction of symmetric holes for non-overgrown holes at Tetch = 390 °C and Tetch = 410 °C. Thus, for the non-overgrown nanoholes, we find at all etching temperatures rather low degrees of symmetry.
In addition to the large degree of asymmetry, we also observe rather large heights h of the surrounding ring structure for non-overgrown nanoholes. For filling of the nanoholes with In0.53Ga0.47As this might act as a diffusion barrier and could possibly affect the adatom mobility of In and Ga atoms differently, which could change the InxGa1−xAs composition inside the nanoholes. The ring height h increases with increasing Tetch. A rather strong change is observed when going from 390 to 410 °C, and for further increased Tetch, the ring height increases only slightly to ∼16 nm at Tetch = 460 °C. In comparison to the GaAs/AlAs system, where the rings around droplet etched holes show heights below 3 nm,13 we observe rather large ring heights with h > 10 nm for Tetch ≥410 °C. Interestingly, the ring height of individual structures is not very homogeneous and fluctuates strongly along the ring. A general trend is that the ring is the highest in the [011]- and [01]-directions. One can only speculate on the material composition of the ring but it might be that the composition is not homogeneous within the ring and, therefore, not lattice-matched to the InP. This would mean the ring material is strained to some degree. This is a significant difference from the GaAs/AlAs system, where the ring, independent of the exact composition, is always unstrained.
We found that overgrowing the nanoholes with In0.52Al0.48As offers a solution to these challenges, as it not only results in a strong reduction of h, but can also allow to improve the fraction of symmetric nanoholes significantly. When overgrowing the holes with In0.52Al0.48As, the holes are basically preserved, especially as the hole depth stays almost constant. The average diameter of the holes increases, especially in the [01]-direction. This means that by overgrowing the holes, the asymmetry is shifted toward an elongation along [01]. This effect becomes more pronounced when the larger thickness dovergrowth of the layer was employed for overgrowing the holes. Averaged values for elongation are listed in Table I. For Tetch = 410 °C, dovergrowth = 100, 150 nm and Tetch = 435 °C, dovergrowth = 150 nm, all measured nanoholes were elongated in [01]. For Tetch = 460 °C, dovergrowth = 0 nm, all, and for Tetch = 460 °C, dovergrowth = 50 nm, all, but one, were elongated in [011].
When starting with non-overgrown nanoholes mainly elongated along the [011]-direction, one can obtain quite symmetric holes by overgrowing with an optimum thickness. This effect led to the increase in symmetric nanoholes for Tetch = 435 °C. Here, we obtain nearly 50% of symmetric nanoholes when overgrowing with dovergrowth = 50 nm, which is due to the improvement of the difference in the diameters along [011] and [01]. We also found improvements in the symmetry for Tetch = 410 °C with overgrowing as well, achieving a fraction of symmetric dots of slightly more than 30%. This is because overgrowing with 50 nm In0.52Al0.48As at Tetch = 410 °C only slightly worsened the elongation in [01], but drastically improved the number of nanoholes that showed an ideal cone-like profile in [011] and [01].
Overgrowing also significantly reduces h and the ring height can even be brought close to zero by overgrowing with 150 nm In0.52Al0.48As. Note that by the overgrowth, any strain that might be present in the original ring structure is strongly reduced at the surface of the overgrown structure. This influences the filling behavior as discussed later. Summarizing, the overgrowth of the holes offers the possibility to improve their symmetry and to reduce the strain in the ring structure in case of non-lattice matched composition. However, one has to accept that the overgrowth approach results in larger hole diameter, and the lateral confinement in a QD generated by filling would be smaller. From the data summarized in Table I, we conclude that dovergrowth = 50 nm is an optimum value. Here, we obtain nearly 50% of symmetric holes. For this reason, we concentrated our studies of the hole filling process on holes overgrown with 50 nm In0.52Al0.48As. Figure 2 shows the AFM images and profiles for selected holes etched at various temperatures and overgrown with 50 nm In0.52Al0.48As. For the further preparation of QD samples, these parameters were selected for In0.53Ga0.47As filling and spectroscopy experiments.
IV. FILLING OF HOLES
Figure 3 shows exemplarily the process of filling holes, which were etched at 410 °C and overgrown with 50 nm In0.52Al0.48As with In0.53Ga0.47As in As4 as well as in As2 atmosphere. The profiles shown are from different samples, i.e., from different nanoholes, but they were selected for being typical representatives from their respective measurement sets. As can be seen, the filling behavior is different, if using As2 or As4, respectively. The process works significantly better with As4, and one can observe a clear filling of the nanoholes with increasing deposition amount, up to complete filling of the holes employing an In0.53Ga0.47As amount corresponding to a homogeneous deposition of 1.4 nm.
Filling of non-overgrown nanoholes using As4 was investigated as well and produced generally a slightly worse filling behavior compared to the overgrown samples, which might be because of the non-overgrown rings being strained due to their composition after the etching process. As we try to avoid strained QDs and as the non-overgrown nanoholes have shown generally lower symmetry, no QD samples with non-overgrown nanoholes were prepared.
While filling with As4 works well, filling under As2 atmosphere appears not to work as well. While 1.4 nm In0.53Ga0.47As deposition completely filled the holes when using As4, with As2, the filling level is less than 50%. Photoluminescence analysis of such a sample with an In0.52Al0.48As capping layer showed no signal from QDs so we concentrated our studies on the filling under As4 atmosphere. AFM images of holes filled with various amounts of In0.53Ga0.47As under As4 and the corresponding profiles are depicted in Figs. 3(c)–3(f). One can see that the ring structure around the holes changes asymmetrically with the deposition of In0.53Ga0.47As. The ring becomes much wider in the [01]-direction, with strongly increasing diameter and slightly increasing height with an increasing amount of In0.53Ga0.47As deposited. In the [011]-direction, the diameter and height of the ring appear to stay roughly the same. We attribute this asymmetric change in morphology of the ring to the difference in diffusion length between the [011]- and [01]-directions, with the adatom mobility being higher in the [01]-direction.33 This leads to an accumulation of (In,Ga)As at the side of the ring and to the elongations of the ring in the [01]-direction. For capped samples, this resulted in additional PL signals at lower wavelengths, which will be discussed below.
V. SPECTROSCOPY
Figure 4(a) shows the PL spectra of samples with three different hole filling levels. All samples have been etched at Tetch = 410 °C. Peaks originating from the QDs formed in the holes are marked in the graph, and the smaller peaks in each spectrum are related to the protective In0.53Ga0.47As layers on top of each sample. These form quantum wells with thickness dependent ground state transition energy so we observe emission at ∼1500 nm for the black and red curve (10 nm thickness) and 1330 nm for the blue curve (5 nm thickness). The QD peaks red-shift with increasing filling levels resulting in a peak at 1350 nm for the deposition of 1.0 nm (corresponding approximately to 10 nm QD height), up to a peak of 1490 nm for the maximally possible filling of 1.8 nm (∼20 nm QD height, i.e., a completely filled hole).
We observe two peaks at higher energies in the PL spectrum (see Fig. S1 in the supplementary material) that red-shift with the amount of deposited In0.53Ga0.47As as well. The first one occurs between 850 and 950 nm (depending on the In0.53Ga0.47As amount), which is due to the In0.53Ga0.47As deposited away from the etched holes. This layer forms a quantum well sandwiched between the two In0.52Al0.48As layers. With increasing In0.53Ga0.47As amount, the thickness of the quantum well increases and the emission red-shifts. In addition, we observe an emission between 900 and 1200 nm. We attribute this emission to the structures formed by the accumulated (In,Ga)As at the sides of the ring structure in the [01]-direction. These are thicker than the quantum well-formed far away from the holes, and therefore, the emission is at a longer wavelength. The emission is quite broad due to the strongly varying sizes and shapes of these structures. The PL spectra for the full range are included in the supplementary material, Fig. S1.
To increase the emission wavelength above 1500 nm without changing the QD or matrix material composition, one has to utilize deeper holes. Figure 4(b) shows the PL measurements of capped samples etched at 435 and 460 °C and completely filled with In0.53Ga0.47As, which was confirmed by control samples without the capping layer measured in AFM (supplementary material, Fig. S2). It can be seen that deeper holes, and in turn larger QDs, result in photon emission above 1500 nm. While the PL peak of the Tetch = 435 °C sample is at 1516 nm, the peak for Tetch = 460 °C red-shifts only slightly to 1524 nm. This means that we are now reaching the limit of increasing the emission wavelength by increasing the QD size. However, from the spectrum, one sees that a significant fraction of the ensemble signal is above 1530 nm, i.e., a significant faction of the quantum dots emits in the optical C-band.
To get more insight into the emission wavelength of the QDs, we performed simple computer simulations of the first two electron and the heavy hole states with the commercial poison solver Nextnano.34 We assumed a circular lens shape with a diameter of 180 nm and a height of 25 nm, which corresponds to the average values of nanoholes produced at Tetch = 435 °C. We assumed the homogeneous composition of In0.53Ga0.47As perfectly lattice matched the surrounding In0.52Al0.48As barrier material. This results in a ground-state emission at 1493 nm, i.e., a little lower as observed experimentally. However, changing the composition inside the QD by 2% to In0.55Ga0.45As red-shifts the simulated QD emission to 1526 nm (strain is included). This indicates that our QDs might not have the perfect lattice matched composition and the indium content is slightly higher than aimed for. A possible explanation is a difference in the diffusion of In and Ga adatoms into the nanoholes, as In generally has a higher surface mobility than Ga.35
To further verify that we have QD emission, we performed single dot spectroscopy. Figures 4(c) and 4(d) show spectra of single dots for the 435 and 460 °C samples, respectively. One clearly sees sharp emission lines in the optical C-band originating from single QDs. The linewidth of 245 μeV is due to the resolution limit of the setup.
VI. SUMMARY
In conclusion, we investigated nanoholes in In0.52Al0.48As layers lattice matched to InP, produced via local droplet etching employing In0.52Al0.48 deposition at various temperatures between Tetch = 390 °C and Tetch = 505 °C. We found very low surface densities of nanoholes, where the densities decrease with increasing etching temperature. The density of holes drops from around 1 × 107 cm−2 for the lowest tested temperature (Tetch = 390 °C), to 4.7 × 105 cm−2 for the highest temperature investigated (Tetch = 505 °C).
This behavior can be quantitatively described by an exponential approach [see Eq. (1)]. Further we found that higher etching temperatures also led to holes with larger depth as well as larger diameter. However, we also observed strong elongation along the [011]-direction when etching above 460 °C and the formation of multiple holes inside a single ring for temperatures over 480 °C. Overgrowing the nanoholes with In0.52Al0.48As under As2 environment preserved the holes, but reduced the height of the surrounding ring and changed the elongation toward the [01]-direction, while increasing the diameter. Most importantly, we found that holes etched at 410 and 435 °C and overgrown with 50 nm In0.52Al0.48As are for our parameters the most promising candidates for symmetric QDs.
The filling of the nanoholes worked best under As4 atmosphere, which might be due lower reactivity of As4 and corresponding better surface mobility of the adatoms. Under the As2 environment, the filling also seems to work but at a much slower rate. For filled nanoholes with In0.52Al0.48As capping, we found ensemble PL signals that red-shift with increasing In0.53Ga0.47As filling amount and originate from the QDs formed in the filled holes. Under optimum conditions, i.e., deep holes and complete filling, we obtained emission in the optical C-band. Single dot spectroscopy shows sharp emission lines with resolution limited linewidth of ∼245 μeV. Nextnano simulation indicated that the QDs formed in the nanoholes might contain slightly more In than the perfectly lattice matched alloy.
Overall, this work presents a promising outlook for strain-free droplet etched QDs emitting at telecom wavelengths, with possible applications as entangled photon sources for quantum communication applications. It also reveals significant quantitative differences to the established GaAs/AlAs system.
SUPPLEMENTARY MATERIAL
See the supplementary material for the full PL spectra of the capped LDE QDs produced at Tetch = 410 °C with dovergrowth = 50 nm and for the AFM images of completely filled nanoholes etched at Tetch = 435 °C and Tetch = 460 °C with dovergrowth = 50 nm. The supplementary material also contains an exemplary SEM measurement of nanoholes etched at Tetch = 435 °C.
ACKNOWLEDGMENTS
The authors acknowledge funding by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) – SFB-Geschäftszeichen Grant No. TRR142/3-2022 – Projektnummer Grant No. 231447078) and co-funded by the European Union (ERC, LiNQs, Grant No. 101042672). Views and opinions expressed are however those of the author(s) only and do not necessarily reflect those of the European Union or the European Research Council. Neither the European Union nor the granting authority can be held responsible for them.
AUTHOR DECLARATIONS
Conflict of Interest
The authors have no conflicts to disclose.
Author Contributions
D. Deutsch: Data curation (lead); Formal analysis (lead); Investigation (equal); Validation (equal); Visualization (lead); Writing – original draft (lead). C. Buchholz: Formal analysis (supporting); Investigation (equal); Validation (equal); Writing – review & editing (equal). V. Zolatanosha: Investigation (supporting); Writing – review & editing (equal). K. D. Jöns: Formal analysis (supporting); Funding acquisition (equal); Supervision (equal); Writing – review & editing (equal). D. Reuter: Conceptualization (lead); Formal analysis (supporting); Funding acquisition (equal); Project administration (lead); Supervision (equal); Writing – review & editing (equal).
DATA AVAILABILITY
The data that support the findings of this study are available from the corresponding author upon reasonable request.