Measuring the hole chemical potential in ferromagnetic Ga 1 x Mn x As Ga As heterostructures by photoexcited resonant tunneling

O. Thomas, O. Makarovsky, A. Patan, L. Eaves, R. P. Campion, K. W. Edmonds, C. T. Foxon, and B. L. Gallagher Citation: Applied Physics Letters 90, 082106 (2007); doi: 10.1063/1.2709624 View online: http://dx.doi.org/10.1063/1.2709624 View Table of Contents: http://scitation.aip.org/content/aip/journal/apl/90/8?ver=pdfcov Published by the AIP Publishing

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APPLIED PHYSICS LETTERS 90, 082106 2007

Measuring the hole chemical potential in ferromagnetic Ga1xMnxAs/ GaAs heterostructures by photoexcited resonant tunneling
O. Thomas, O. Makarovsky, A. Patan,a L. Eaves, R. P. Campion, K. W. Edmonds, C. T. Foxon, and B. L. Gallagher
School of Physics and Astronomy, University of Nottingham, Nottingham NG7 2RD, United Kingdom

Received 21 December 2006; accepted 22 January 2007; published online 23 February 2007 The authors investigate the optical and electrical properties of a p-i-n GaAs/ AlAs resonant tunneling diode in which the p-type layer is the ferromagnetic alloy semiconductor Ga1xMnxAs x = 3 % . The high density of Mn acceptors affects signicantly the electrostatic potential prole of the heterostructure and inhibits hole tunneling from Ga1xMnxAs.The authors use photoconductivity to probe this potential and measure the hole chemical potential in Ga1xMnxAs relative to the band edges of the adjacent undoped GaAs layers. 2007 American Institute of Physics. DOI: 10.1063/1.2709624 The dilute ferromagnetic semiconductor alloy Ga1xMnxAs has emerged as a candidate material system for applications in spintronics.14 Substitutional Mn in GaAs MnGa is an acceptor impurity with a hole binding energy of 110 meV.5 At high Mn concentrations, the acceptor impurity band tends to merge with the valence band. Hence the holes become mobile, even at low temperatures, and act as itinerant carriers of the ferromagnetic interaction between the 2+ ions.1,6,7 A Curie temperature of up to 173 K has reMnGa cently been achieved.8 At present there is no rm consensus concerning the dependence on Mn content of the energy gap of Ga1xMnxAs and the location of the chemical potential p relative to the conduction and valence band edges. Optical spectroscopy measurements9 indicate that for high x x = 5 % 7 % , p lies within the Mn-impurity band. Room temperature scanning tunneling microscopy has measured a band gap of 1.23 0.05 eV for x 3%.10 A knowledge of these material parameters is essential for the design, modeling, and operation of Ga1xMnxAs heterostructure devices, including p-i-n light-emitting diodes. In this type of device, spin-polarized holes can be injected from Ga1xMnxAs into the intrinsic i region of the diode to give polarized electroluminescence EL emission.3 In this letter we investigate the electronic and optical properties of a p-i-n double barrier resonant tunneling diode RTD incorporating an AlAs/ GaAs/ AlAs quantum well QW and a p-doped Ga1xMnxAs layer with x = 3%. The high density of Mn acceptors in the p-type layer affects signicantly the electrostatic potential prole of the diode and inhibits the injection of holes from Ga1xMnxAs. Photoconductivity PC measurements allow us to probe the potential prole and to locate precisely the position of the chemical potential in Ga1xMnxAs with respect to the band edges in the adjacent GaAs layers. This information is particularly useful as it determines the bias required for hole injection into the QW subbands. The sequence of layers, grown by molecular beam epitaxy on 100 semi-insulating GaAs substrates, is as follows see inset of Fig. 1: a 300 nm Si-doped GaAs layer n = 2 1018 cm3; 100 nm of Si-doped GaAs n = 2
a

1017 cm3; an undoped intrinsic i region consisting of a 20 nm GaAs spacer layer, a 6 nm GaAs QW formed between two 5 nm AlAs barriers, and a 10 nm GaAs spacer layer; the top 50 nm Ga1xMnxAs layer with x = 3% was grown at 250 C. We have also studied a control sample of similar design, except that the Ga1xMnxAs layer was replaced by a 1 m layer of carbon-doped GaAs p = 2 1018 cm3. The layers were processed into 200 m diameter mesa diodes with a ring-shaped electrode on the top of the mesa for EL and for current-voltage, IV, measurements under optical excitation with the 633 nm line of a HeNe laser. We have studied annealed and unannealed devices. Annealing has been shown to signicantly reduce compensation in Ga1xMnxAs through Mn interstitial outdiffusion11 and can lead to hole densities close to the Mn concentration of 6.6 1020 cm3 for x = 3%.12 In this work, we only consider samples that were unannealed or else annealed only for short

Author to whom correspondence should be addressed; electronic mail: amalia.patane@nottingham.ac.uk

FIG. 1. Low-temperature T = 4.2 K IV curve of the p-i-n diode containing the p-Ga1xMnxAs layer upper curve and of the control sample in which the p layer is doped with shallow carbon acceptors bottom curve. The inset is a sketch of the layer composition of the p-i-n diode containing the p-Ga1xMnxAs layer.

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FIG. 2. a Low-temperature T = 12 K EL spectrum for the p-i-n diode containing the p-Ga1xMnxAs layer V = 1.89 V. b Bias dependence of the EL intensity for the QW emission circles and of the tunnel current solid line.

times 3 h at relatively low temperatures T = 150 C. Under these annealing conditions, only limited outdiffusion of compensating Mn interstitials will occur, and a hole density of around 4.1 1020 cm3 is expected.12,13 Figure 1 compares the low-temperature T = 4.2 K IV curve of the p-i-n diode containing the p-Ga1xMnxAs layer The steplike increase of the QW EL emission Fig. 2b with that of the control sample in which the p layer is doped just beyond the E1 peak demonstrates that hole injection with shallow carbon acceptors. For the control sample, the from the Ga1xMnxAs p layer into the QW is controlled by strongest peak in IV corresponds to electron tunneling into the electron current. In addition, the absence of hole resothe lowest conduction subband E1; the three weaker peaks, nances in IV Fig. 1 indicates that the current is dominated HH1, LH1, and HH2, arise from resonant hole tunneling,14,15 by electron tunneling. To understand this unusual behavior where LHn and HHn refer to QW subbands with light L or we consider the effect of the high density of Mn acceptors on heavy H hole character at wave vector k = 0 and n = 1 , 2 is the electrostatic potential prole of the diode. Figure 3a the subband quantum number. In contrast, the diode incorposhows a schematic diagram of the band edges of the heterorating the Ga1xMnxAs layer reveals only a single resonance structure at a voltage VFB corresponding to the atband conin IV due to electron tunneling into E1. dition at which the electric eld in the intrinsic region is As shown in Fig. 2, the low-temperature T = 12 K EL zero. In this diagram, we assumed that the band gap of spectrum of the diode containing the p-Ga1xMnxAs layer Ga1xMnxAs is smaller than that of GaAs, as indicated by consists of a strong band around 1.50 eV arising from excirecent experiments.10 The potential step at the interface be0 tonic X and carbon-acceptors-related e-C recombination tween Ga1xMnxAs and the GaAs spacer layer is made up of in the GaAs layers and a sharp line at 1.65 eV involving two contributions: a the band-edge discontinuity due to the radiative transitions between the edges of the quantized subsmaller band gap of Ga1xMnxAs and b the dipolar charge bands E1 HH1 of the QW. The weaker features around at the edge of the Ga1xMnxAs layer created by negatively 1.4 eV are due to recombination of electrons with holes ionized Mn acceptors and holes which diffuse into GaAs. bound to residual Mn acceptors in the GaAs layers e-Mn0. Since the chemical potential on the n-type side of the barriers The EL from the QW has a weak circular polarization is very close within a few meV to the energy Ec of the 1 % , which will be discussed in a subsequent article. This GaAs conduction band edge, at V = VFB the hole chemical emission indicates that holes are injected into the QW from potential in Ga1xMnxAs lies at a well-dened energy the p-Ga1xMnxAs layer despite the absence of discernible p = eVFB below Ec in the adjacent GaAs layers, see hole resonances in IV. As shown in Fig. 2b, the QW EL Fig. 3a. peak intensity increases sharply at 1.85 V corresponding to For V VFB, hole injection from Ga1xMnxAs into the the fall in current just beyond the E1 peak in IV. In conQW is inhibited by the potential step at the Ga1xMnxAs-spacer layer interface. Hence the current is trast, the bias dependence of the QW EL intensity of the 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: 1.209.174.47 dominated by resonant transmission of electrons through E1, control sample follows closely that of the tunnel current.15
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FIG. 3. a Schematic diagram of the conduction and valence band edges of our p-i-n diode containing the p-Ga1xMnxAs layer biased at V = VFB for which the electric eld in the intrinsic region of the device is zero. b Schematic of the dynamics of photoexcited electrons and holes when the diode is biased at V VFB. c Low-temperature T = 4.2 K IV characteristics for different intensities of laser excitation P = 0, 4, 11, 18, and 35 W cm2. The inset shows the hole and electron resonances in the differential conductance, dI / dV, plot for Pmax = 35 W cm2. The right insets show the intersection point, VFB, in photocurrent for our p-i-n diode containing the p-Ga1xMnxAs layer top inset and for our control sample in which the p-type GaAs layer is doped with shallow carbon acceptors bottom inset.

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as is evident from Fig. 1. These electrons recombine with holes in the Ga1xMnxAs and GaAs layers on the p side of the diode, thus reducing further the density of holes near the barrier that are available for tunneling into the QW. However, when the electron tunnel current falls beyond the E1 peak, the number of available holes increases, leading to the sharp rise of the QW EL intensity at 1.85 V shown in Fig. 2b. A key parameter of our Ga1xMnxAs heterostructure is the hole chemical potential energy p, which we derive from the bias dependence of the PC response at T = 4.2 K. For V VFB, the photocreated electrons and holes are swept by the electric eld in opposite directions and form accumulation layers adjacent to the tunnel barriers, see Fig. 3b. Since the dark current is negligible for V VFB, the current measured under illumination is due to the photocreated carriers tunneling through the barriers. The photocurrent is zero at the atband condition, i.e., when V = VFB = p / e, from which we determine the position of p. The PC response of the Ga1xMnxAs diode exhibits a negative photocurrent at biases below VFB = 1.410 V and a resonant peak at V = 1.18 V, see Fig. 3c. The IV curves measured under different excitation powers all intersect at VFB at which the photocurrent is zero. We observe a similar PC effect in our control sample, but the intersection point occurs at a signicantly higher bias, VFB = 1.514 V see right insets of Fig. 3c. This corresponds to p = 1.514 0.005 eV, which as expected, is close to the band gap of pure GaAs at T = 4.2 K Eg = 1.519 eV. The corresponding energy for the Ga1xMnxAs diode is considerably smaller, p = 1.410 0.005 eV. Hence, we deduce that there is an interface barrier of height Uh = Ev p = 0.11 eV between holes at p in the Ga1xMnxAs layer and the valence band edge, Ev = 1.519 eV, in the adjacent GaAs layers. This barrier explains the absence of distinct hole resonant tunneling peaks in the dark IV curve of our Ga1xMnxAs diode and may be also relevant to the observation of highly asymmetric resonant tunneling peaks in the IV curves of p-i- p Ga1xMnxAs RTDs.16 A similar barrier height was derived from thermionic emission data in p-i- p Ga1xMnxAs diodes with x = 1.4% 5.1%.17 We note that our value of p coincides with that of the ground state of the isolated substitutional Mn acceptor impurity in GaAs,5 thus indicating that the chemical potential remains pinned to this level as the Mn concentration changes from the dilute to the alloy regime. Finally, we consider the resonant features in the bias region where the PC is negative. We attribute the peak at 1.18 V to resonant tunneling of the photocreated electrons from the accumulation layer at the right hand barrier through the E1 subband of the QW and into the n-doped contact layer. The current path is completed by the diffusion of the photoexcited holes towards the Ga1xMnxAs layer, see Fig. 3b. A similar process involving resonant tunneling of photocreated holes from the accumulation layer into the HH1 and HH2 QW subbands gives rise to two weak resonant features in the differential photoconductance plot, dI / dV, see

inset of Fig. 3c. The presence of these hole resonances in photoexcitation and their absence in the dark current for V VFB is further evidence that hole injection into the QW from the Ga1xMnxAs layer is inhibited by a potential barrier at the Ga1xMnxAs-spacer layer interface. In conclusion, we have studied a p-i-n light-emitting resonant tunneling diode in which the p-type hole emitter is Ga1xMnxAs x = 3 % . The incorporation of Mn leads to a signicant modication of the electronic band properties. Photoconductivity measurements as a function of bias provide a means of determining precisely the position of the hole chemical potential in the Ga1xMnxAs layer with respect to the band edges in adjacent GaAs layers. This information should be of use in the design and study of spintronic devices involving hole injection from ferromagnetic Ga1xMnxAs. The work is partly supported by EPSRC U.K.. The authors thank D. Taylor and J. Chauhan for processing our devices.
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