Tunneling carrier escape from InAs self-assembled quantum dots J. Ibáñez, R. Leon, D. T. Vu, S. Chaparro, S. R. Johnson, C. Navarro, and Y. H. Zhang Citation: Applied Physics Letters 79, 2013 (2001); doi: 10.1063/1.1402642 View online: http://dx.doi.org/10.1063/1.1402642 View Table of Contents: http://scitation.aip.org/content/aip/journal/apl/79/13?ver=pdfcov Published by the AIP Publishing Articles you may be interested in Multiexciton complexes in InAs self-assembled quantum dots J. Appl. Phys. 105, 122406 (2009); 10.1063/1.3117231 Effect of In–Ga intermixing on the electronic states in self-assembled InAs quantum dots probed by nanogap electrodes Appl. Phys. Lett. 94, 162107 (2009); 10.1063/1.3123816 High Kondo temperature ( T K ∼ 80 K ) in self-assembled InAs quantum dots laterally coupled to nanogap electrodes Appl. Phys. Lett. 93, 062101 (2008); 10.1063/1.2968206 Combined optical and electrical studies of the effects of annealing on the intrinsic states and deep levels in a self-assembled InAs quantum-dot structure J. Appl. Phys. 100, 043703 (2006); 10.1063/1.2234817 Controlling the electron tunneling through InAs self-assembled dots J. Appl. Phys. 91, 3474 (2002); 10.1063/1.1446226 This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: 209.147.144.21 On: Tue, 10 Feb 2015 00:35:25 APPLIED PHYSICS LETTERS VOLUME 79, NUMBER 13 24 SEPTEMBER 2001 Tunneling carrier escape from InAs self-assembled quantum dots J. Ibáñez,a) R. Leon, and D. T. Vu Jet Propulsion Laboratory, California Institute of Technology, 4800 Oak Grove Drive, Pasadena, California 91109 S. Chaparro, S. R. Johnson, C. Navarro, and Y. H. Zhang Center for Solid State Electronic Research, Arizona State University, Tempe, Arizona 85287 共Received 20 April 2001; accepted for publication 13 July 2001兲 Deep-level transient spectroscopy measurements in InAs quantum dots 共QDs兲 grown in both n-GaAs and p-GaAs show that tunneling is an important mechanism of carrier escape from the dots. The doping level in the barrier strongly affects the tunneling emission rates, enabling or preventing the detection of a transient capacitance signal from a given QD level. The relative intensity of this signal acquired with different rate windows allows the estimation of tunneling emission energies. © 2001 American Institute of Physics. 关DOI: 10.1063/1.1402642兴 Stranski–Krastanow quantum dots 共QDs兲 have recently attracted much attention due to their unique optical and electronic properties, which are enabling a wide range of novel applications.1 The transition energies between QD electron and hole levels can be directly measured from photoluminescence 共PL兲 peaks. However, PL provides little information on electron and hole levels relative to the barrier band edges. Space charge techniques such as capacitance–voltage spectroscopy (C – V) 2–5 and deep-level transient spectroscopy 共DLTS兲6 –9 allow absolute positioning of the QD levels, providing complementary information to PL. Carrier capture and escape dynamics of the dots can also be studied by means of DLTS. There has been some discrepancy between different published works on DLTS in the extensively studied InAs/GaAs self-assembled QDs. Direct measurements of the energy difference between the dot levels and the energy band of the barrier7 have been reported, while other works show evidence of capture barriers into the dots.8 The possibility that some of the DLTS signals detected are originated from traps near the dots has also been suggested.9 To this day, only one study has reported clear detection of electron escape by means of tunneling in InAs QDs.7 In the present work, DLTS measurements performed on InAs QDs embedded in n- and p-GaAs show that tunneling is an important escape mechanism in quantum dots. Tunneling emission rates and energies are estimated by means of C – V and DLTS. QD structures were grown by molecular beam epitaxy. Two samples with eight 50-nm layers of n-type 共p-type兲 GaAs (n⫽p⫽1017 cm⫺3) terminated with InAs QDs 共⬃2 ML coverage兲 were grown over a 300-nm-thick, n ⫹ -doped GaAs buffer layer. A final GaAs capping layer with the same doping level was deposited. A top Schottky diode and back ohmic contacts were formed for the n-type sample, and back and top ohmic contacts were formed on the p-type sample. The DLTS measurements were carried out at delay times ␶ in the 共0.02–1000兲 ms range and at a rate window10 of 4.3⫻ ␶ . Analysis of island sizes and densities using atomic force Present address: Institut Jaume Almera 共C.S.I.C.兲, Barcelona, Spain. a兲 microscopy in air give average diameters of 40 nm, 5 nm heights, and concentrations of 3⫻1010 cm⫺2 for uncapped QDs grown under the same conditions. PL spectra for these structures were obtained at 300 and 77 K using an Ar⫹ laser for excitation and a cooled Ge detector with lock-in techniques for signal detection. The extrapolated ground state emission at 4 K is ⬃1.15 eV, with full width at half maximum ⬃130 meV. A typical C – V profile obtained at 75 K for the n-type sample is shown in curve A 共filled circles兲 of Fig. 1. Three plateaus corresponding to three different layers of dots are observed in addition to the background capacitance from the doped GaAs layers. Since only one plateau per QD level is expected,2 we attribute each plateau to the emptying of a single QD level. Curve C 共filled circles兲 of Fig. 1 shows a similar behavior for the p-type sample. High leakage current for this sample allows biasing only to 2 V, therefore, only two plateaus were observed. Models of different level of sophistication have been used to study the C – V profile of single QD layers.3,5 A simpler analysis of the C – V profile is possible by calculating the charge in the dots as a function of the applied voltage by using the expression reported in Refs. 3–5 for the density of electron states in the QD sheet but assuming that the FIG. 1. Capacitance–voltage profile at 75 K for n-InAs QDs 共curve A, filled circles兲 and p-InAs QDs 共curve C, filled circles兲. Calculated C – V profiles are shown as solid curves. Curve B shows DLTS-signal intensity vs reverse bias at 20 K for the n-type sample. The dashed line is a guide to the eye. This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: 0003-6951/2001/79(13)/2013/3/$18.00 2013 © 2001 American Institute of Physics 209.147.144.21 On: Tue, 10 Feb 2015 00:35:25 2014 Ihár̃ez et al. Appl. Phys. Lett., Vol. 79, No. 13, 24 September 2001 FIG. 2. DLTS spectrum ( ␶ ⫽0.02 ms) for the n-type InAs-QD sample 共open circles兲, for biasing conditions ⫺0.75 V/⫺0.05 V, and for the p-type InAs QDs 共filled circles兲, for biasing conditions ⫺0.75 V/⫺0.05 V ( ␶ ⫽5 ms). The inset shows the intensity of the flat signal at 20 K for the n-type 共open circles兲 and the p-type samples 共filled circles兲 vs delay time. depletion-region approximation still holds. The total capacitance is then given by the QD-related capacitance plus the background capacitance. This method, already applied using a lever-arm relation for a single layer of dots in Ref. 4, facilitates the calculation for a multilayered system. Within this approach we obtain the best fit 共solid line兲 to curve A of Fig. 1 when one QD level with energy E n ⫽250 meV below the GaAs conduction band and energy dispersion ⌬E n ⫽140 meV is taken into account. For the p-type sample we obtain the best fit 共solid line兲 to curve C with one single QD level with energy E p ⫽110 meV above the GaAs valence band and energy dispersion ⌬E p ⫽140 meV. Figure 2 共open circles兲 shows a DLTS spectrum for the n-type sample, consisting of a quasiflat signal that extends over the whole range of temperatures. A DLTS peak 共not shown in the graph for scaling reasons兲 with an activation energy of 0.40 eV appears for higher temperatures. Since this peak was only detected for positive or low negative filling biases, we believe it to be related to deep surface traps and not to the dots. The spectrum for the p-type sample 共filled circles兲 shows a flat signal for the lower temperatures, and a step-like reduction to zero signal at about 55 K. To understand both spectra we must take into account that two carrierescape mechanisms exist: thermal escape and tunneling. In the former, the quantum dot behaves like a deep trap and hence its thermal emission rate e th is given by e th ⫽AT 2 exp(⫺Ea /KT), where E a is the activation energy of the QD level and A is a temperature-independent constant proportional to the capture cross section.10 On the other hand, assuming a triangular barrier for the carriers trapped in the QDs, the tunneling escape rate can be written as11 intensity of this signal depends on the tunneling emission rate and the rate window. For sufficiently high temperatures, thermal emission dominates, giving rise to a step-like reduction of the tunneling flat signal at the temperature of the DLTS peak that would be present in the absence of carrier escape by tunneling. This allows estimating the activation energy of QD levels by Arrhenius plots, determining the position of the step for different rate windows. The lowtemperature flat signal obtained for the p-type sample originates by hole tunneling escape from the dots, whereas the reduction to zero signal at about 55 K arises from thermal escape. We obtain a value of 100⫾20 meV for the activation energy of the QD hole level, which is in good agreement with the C – V results. Slight variations of this value are obtained depending on the applied reverse bias, which can be explained by variations of the energy level of the dots due to the electric field. No step-like reduction is detected for the n-type sample 共open circles in Fig. 2兲 up to 325 K because the DLTS signal detected at higher temperatures hinders any other feature. The inset of Fig. 2 plots the intensity of the flat signal at 20 K for both the n-type and the p-type samples as a function of the delay time. For the n-type sample, the flat signal is detected with the lowest rate window available 共delay time of 0.02 ms兲. For the next wider rate windows 共delay times of 0.05 and 0.1 ms兲 the flat signal detected is strongly reduced, which is a consequence of high rate of electron escape by tunneling. For the next rate windows available, no signal at all is detected. To further confirm that the flat signal obtained for the n-type sample is originated by electrons escaping from the dots, we have measured its intensity at 20 K versus applied reverse bias. A positive filling bias was used to include the first layer of dots. The result, plotted in Fig. 1 共curve B兲, shows three plateaus that coincide with the plateaus of the C – V measurement 共curve A兲. The intensity of the flat signal increases when the applied reverse bias is sufficient to include a given layer of dots. For higher reverse bias the tunneling escape rate increases due to the increase of the electric field, and this diminishes the intensity of the flat signal. For a carrier captured in a QD level to escape, the level must be above the Fermi energy in the barrier region. This happens for a certain onset reverse bias V c that, within the depletion approximation, satisfies the relation ⫺q ␺ (V c ) ⫹E h ⫽q(V c ⫹ ␺ 0 )⫺E F , which leads to 冉 冊 E h ⫺q 共 V c ⫹ ␺ 0 兲 1⫺ L W 2 ⫹E F ⫽0, 共2兲 where ␺ (V c ) is the potential at the dot layer, E F is the Fermi energy at the barrier, W⫽ 关 2( ␺ 0 ⫹V c ) ⑀⑀ 0 /qN A,D 兴 1/2 is the depletion-region width, L is the distance from the dots to the diode junction, N A,D is the doping level at the barrier and ␺ 0 is the built-in potential. For this voltage V c , the electric field qF 4 共 2m * 兲 1/2E 3/2 h F at the dots can be calculated using the depletion approxie tun⫽ , 共1兲 1/2 exp ⫺ 4 共 2m * E h 兲 3 qបF mation. By inserting the value of F into Eq. 共1兲, the lowest where E h is the barrier height, F is the electric field at the emission energy that gives rise to tunneling rates detectable dot, q is the electron charge, and m * is the effective mass of with the shortest rate window available 共delay time of 0.02 the carriers in the energy band of the barrier material. For ms兲 can be calculated. A lower emission energy would yield sufficiently low temperatures, the total emission rate e n carrier escape rates too fast to be detected with our instru⫽e th⫹e tun is dominated by tunneling, which is temperature mentation. We calculate that our lowest experimentally deThis article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: independent and therefore yields a flat DLTS signal. The tectable emission energy is about 0.17 eV for electrons, 冉 冊 209.147.144.21 On: Tue, 10 Feb 2015 00:35:25 Ihár̃ez et al. Appl. Phys. Lett., Vol. 79, No. 13, 24 September 2001 TABLE I. QD energy level obtained by C – V measurements 共first column兲, compared with activation energy E a 共second column兲 and barrier height E h 共third column兲 obtained from DLTS. InAs/n-GaAs QDs InAs/p-GaAs QDs E n,p Ea Eh 0.25 eV 0.11 eV ¯ 0.10 eV 0.27 eV 0.13 eV about 0.15 eV for light holes, and about 0.060 eV for heavy * ⫽0.076 and holes. We have used the values m e* ⫽0.068, m lh * ⫽0.50 for the effective mass of the different carriers.12 m hh Hence, the doping level in the n-type barrier does not allow detection of DLTS signals from shallower QD electron levels 共higher-energy excited states measured by PL兲. For the p-type sample, we attribute the DLTS signal obtained to tunneling from a heavy hole level, since its emission energy is of about 0.10 eV, whereas no light hole levels lower than 0.15 eV can be observed for the experimental conditions of this work. Different results reported in the literature on InAs QDs could be accounted for by different doping levels in the GaAs matrix. Additional investigation on samples with different doping levels should be performed. Finally, it is possible to evaluate the tunneling emission energy by measuring the relative intensity of the tunnelingrelated flat signal of two different DLTS spectra acquired with two different rate windows, defined by the time intervals (t 1 ,t 2 ) and (t 1⬘ ,t 2⬘ ), respectively.10 The relative intensity of these tunneling signals is given by exp共 ⫺e tunt 2 兲 ⫺exp共 ⫺e tunt 1 兲 I ⫽ . I ⬘ exp共 ⫺e tunt 2⬘ 兲 ⫺exp共 ⫺e tunt ⬘1 兲 2015 the energy values that we calculate would be average values of the QD levels involved. Whereas C – V provides information about discharging of the QD levels with respect to the position of the Fermi energy, DLTS provides information about the barrier that the carriers must overcome to escape. It should be noted that the sum of the hole and electron energy levels determined with C – V and DLTS plus the ground-state recombination energy for the dots studied in this work 1.15 eV at 4 K兲 is close to the GaAs band gap 1.52 eV at 4 K兲. This fact and the closeness of the QD-level energies obtained by C – V and DLTS do not support the concept of capture barriers for the carriers into these QDs. This is in agreement with previous results on temperature-dependent PL14 and time-resolved PL experiments,15 in which important capture barriers have only been identified in low-density QDs, but not in high-density QDs like those studied here. In conclusion, DLTS signals detected from InAs QDs are strongly affected by carrier escape by tunneling, with escape rates strongly dependent on the doping density of the barrier. The tunneling emission energies do not support the existence of high capture barriers into these QDs. The authors thank Salvador Dueñas for providing calibration samples, and Ken Evans for valuable experimental input. This work was carried out by the Jet Propulsion Laboratory, California Institute of Technology, under a contract with the National Aeronautics and Space Administration. One of the authors 共J.I.兲 acknowledges the Spanish Ministerio de Educación y Cultura for financial support. 共3兲 The emission energy can then be evaluated by using Eq. 共1兲 with the value of e tun obtained from Eq. 共3兲. With this procedure, and using the data for the n-type sample plotted in the inset of Fig. 2, we estimate tunneling emission times for the n-type sample in the 共20–50兲 ␮s range, which leads to an emission energy of 0.27⫾0.04 eV which is close to the value obtained by C – V. For the p-type sample, we estimate tunneling times between 共30 and 500兲 ␮s, which gives rise to an emission energy of 0.13⫾0.03 eV, again, close to the value obtained with the C – V analysis. This value is also close to the value 0.10⫾0.02 eV obtained for the activation energy using the position of the step-like reduction in the spectra of the p-type sample. Table I displays the different energy values for the electron 共hole兲 levels relative to the GaAs conduction 共valence兲 band obtained in this work. The proximity of energy values determined with different procedures seems to indicate that both the low-temperature flat signal and the step originate from the same QD level, in contrast to the two-level escape mechanism proposed in Ref. 7. Although Coulomb charging effects prevent the observation of higher excited states by space charge techniques,13 it is possible that two or even more QD levels close in energy are responsible for the C – V and DLTS spectra obtained here. In this case, 1 D. Bimberg, M. Grundmann, and N. N. Ledentsov, Quantum Dot Heterostructures 共Wiley, Chichester, 1998兲. 2 G. Medeiros-Ribeiro, D. Leonard, and P. M. Petroff, Appl. Phys. Lett. 66, 1767 共1995兲. 3 P. N. Brounkov, A. Polimeni, S. T. Stoddart, M. Henini, L. Eaves, P. C. Main, A. R. Kovsh, Yu. G. Musikhin, and S. K. Konnikov, Appl. Phys. Lett. 73, 1092 共1998兲. 4 A. J. Chiquito, Yu. A. Pusep, S. Mergulhão, J. C. Galzerani, and N. T. Moshegov, Phys. Rev. B 61, 5499 共2000兲. 5 R. Wetzler, A. Wacker, E. 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