Mn enriched surface of annealed (GaMn)As layers annealed under arsenic capping M. Adell, J. Adell, L. Ilver, and J. Kanski Department of Applied Physics, Chalmers University, of Technology, SE-412 96 Göteborg, Sweden J. Sadowski and J. Z. Domagala Institute of Physics, Polish Academy of Sciences, al. Lotnikow 32/46, 02-668 Warszawa, Poland Received 3 August 2006; published 22 February 2007 Using synchrotron radiation based spectroscopic methods we have investigated the surface modifications of Ga 1-x Mn x As layers due to post growth annealing under amorphous arsenic capping layers. It is established that there is a clear increase of the Mn concentration at the surface after annealing. This is ascribed to a reaction between diffusing Mn interstitials and the As capping. The reacted surface is smooth and well ordered with a 1 2 reconstruction. All data indicate that the annealed GaMnAs is terminated by a monolayer MnAs in zinc-blende structure. DOI: 10.1103/PhysRevB.75.054415 PACS numbers: 75.50.Pp, 79.60.Bm I. INTRODUCTION Since the discovery of ferromagnetism in GaMnAs, 1 this system has become a test ground for development of deeper insight into the mechanisms that control the magnetic prop- erties of diluted magnetic semiconductors. In the perspective of future spintronics applications GaMnAs has an obvious advantage over other candidate systems: it is compatible with the well-developed III-V technology and can therefore be easily integrated into a whole range of optoelectronics. In addition, already the as-grown GaMnAs has a remarkably high ferromagnetic transition temperature 60–80 K 13 as compared to only a few K, e.g., for II-VI based materials. 4 To be of practical use, however, the material must maintain its ferromagnetic properties above room temperature. Much of the ongoing research is thus aiming in this direction. It has been shown by several groups that the Curie tem- perarure T c of GaMnAs films can be considerably in- creased by post growth thermal treatment, 58 from typically 60–80 K up to 160–170 K. However, these desired effects were achieved only when the free surface was exposed to air or nitrogen atmosphere. It was also found that protective GaAs capping layers suppressed the annealing induced modifications. These observations strongly suggested that the annealing effects are associated with a surface reaction, and it is therefore natural to assume that the process involves out-diffusion and passivation of Mn interstitials Mn I . Due to a tendency to compensate the increasing Mn Ga -induced p-doping and also as a result of the low-temperature growth, the density of n-type defects Mn I and As Ga is abundant in GaMnAs. The Mn I are, however, highly mobile at tempera- tures comparable with the GaMnAs growth temperature. 9,10 The removal of Mn I by annealing is reflected via a consid- erably increased density of uncompensated carriers 8 and a reduced lattice constant. 11 A serious limitation of the above-mentioned annealing procedures is that the treated layers are not useful for further processing. The reacted surfaces are disordered and cannot be restored due to the metastable character of the material. To get around this problem, we recently devised an alterna- tive method of annealing. 12 The treatment is in this case car- ried out in the MBE growth chamber, where the reactive medium oxygen or nitrogenis replaced by a 1000 Å thick surface layer of amorphous As deposited at a sample temperature close to room temperature. The method is ex- tremely efficient for removing the interstitial Mn, and the resulting surface is well-ordered. Depending on the experi- mental conditions, this preparation can result in either an atomically smooth surface, suitable for further epitaxial growth, or a surface covered with self-organized quantum dots. 13 In the present paper the first type of surfaces have been characterized with respect to their composition and electronic properties. For the sake of completeness we also discuss Hall effect, x-ray diffraction and magnetization data, all obtained on samples annealed in air, but with an As cap. Obviously, as long as the capping is sufficiently thick, it is irrelevant whether the annealing is carried out in situ or ex situ. II. EXPERIMENT The experiments were performed at the Swedish national synchrotron radiation facility MAX-lab. The GaMnAs films were prepared in a KRYOVAK MBE system, attached to the photoelectron spectrometer at beamline 41 at the MAX I storage ring. This growth system is equipped with five stan- dard Knudsen effusion cells and one valved cracker source for As 2 deposition. The substrates were 1 1 cm 2 pieces of n-doped epiready 001GaAs, indium glued to transferable Mo substrate holders. During growth the sample temperature was monitored by an IR pyrometer, covering the temperature range 100 °C–700 °C, i.e., both the high temperatures HT, 600 °C, used for regular GaAs growth and the low temperatures LT, 230 °C, used for LT-GaAs and GaMnAs growth. This pyrometer was also used to monitor the sample temperature during the annealing treatments per- formed in situ. The samples studied here were all annealed at 180 °C. A 10 keV RHEED system is used for monitoring the sample surface during the growth. The growth rate and concentration of substitutional Mn, Mn Ga , was determined by means of RHEED oscillations, which persisted for ex- tended time despite the extreme growth conditions. 3 In cases PHYSICAL REVIEW B 75, 054415 2007 1098-0121/2007/755/0544156©2007 The American Physical Society 054415-1