We determined the lattice location of Mn in ferromagnetic (Ga,Mn)As using the electron emission channeling technique. We show that interstitial Mn occupies the tetrahedral site with As nearest neighbors (T As ) both before and after thermal annealing at 200 °C, whereas the occupancy of the tetrahedral site with Ga nearest neighbors (T Ga ) is negligible. T As is therefore the energetically favorable site for interstitial Mn in isolated form as well as when forming complexes with substitutional Mn. These results shed new light on the long standing controversy regarding T As versus T Ga occupancy of interstitial Mn in (Ga,Mn)As.[http://dx.doi.org/10.1063/1.4905556] a lino.pereira@fys.kuleuven.be (Ga,Mn)As has become the model system, in which to explore the physics of carrier-mediated ferromagnetism in semiconductors and the associated spintronic phenomena.
1,2In particular, as the most widely studied dilute magnetic semiconductor (DMS), (Ga,Mn)As is the perfect example of how the magnetic behavior of DMS materials is strongly influenced by local structure. In typical high Curie temperature (T C ) (Ga,Mn)As thin films (several % Mn regime), the majority of the Mn atoms substitute for Ga (Mn s ), while a minority fraction (several % of all Mn) occupies interstitial sites (Mn i ).3,4 Mn s provides both the localized magnetic moment and the itinerant hole that mediates the magnetic coupling, whereas Mn i has a twofold compensating effect: (i) magnetically, as Mn i -Mn s pairs couple antiferromagnetically and (ii) electrically, since double donor Mn i compensates Mn s acceptors.3 For a given Mn s concentration, Mn i therefore determines the hole concentration, the Fermi level and the effective Mn s concentration (of non-compensated Mn s moments), all of which define the magneto-electronic behavior of (Ga,Mn)As. The existence of such a crucial role of Mn i is clearly reflected in the effect of the Mn i concentration on the two relevant figures of merit: T C and magnetization. 3−5 Despite this central role in the understanding of (Ga,Mn)As, and, consequently, of Mn-doped III-V DMS materials, interstitial Mn is far from being a well understood defect. The presence of Mn i in ferromagnetic (Ga,Mn)As was first reported based on ion channeling measurements.
6Although consistent with Mn i occupying tetrahedral (T) interstitial sites, the measurements did not allow to discriminate between the two nonequivalent T sites: coordinated by four Ga atoms (T Ga ) or by four As atoms (T As ). Transmission electron microscopy measurements using the (002) diffracted beam indicated that Mn i predominantly occupies the T As site.7 X-ray absorption fine structure (XAFS) techniques were later applied, suggesting T Ga occupancy (e.g., Refs. 8 and 9). However, XAFS is not well suited to distinguish neighboring elements with similar atomic numbers, as is the case for Ga and As, especially in such cases of multi-site occupancy (substitutional and interstitial), where the site to be identified is in fact the minority one (interstitial). In pi...