Donor-vacancy complexes in Ge: Cluster and supercell calculations J. Coutinho, 1 S. Öberg, 2 V. J. B. Torres, 1 M. Barroso, 1 R. Jones, 3 and P. R. Briddon 4 1 Department of Physics, University of Aveiro, Campus Santiago, 3810-193 Aveiro, Portugal 2 Department of Mathematics, Luleå University of Technology, Luleå S-97187, Sweden 3 School of Physics, University of Exeter, Exeter EX4 4QL, United Kingdom 4 School of Natural Sciences, University of Newcastle upon Tyne, Newcastle upon Tyne NE1 7RU, United Kingdom Received 20 March 2006; published 26 June 2006 We present a comprehensive spin-density functional modeling study of the structural and electronic prop- erties of donor-vacancy complexes PV, AsV, SbV, and BiVin Ge crystals. Special attention is paid to spurious results which are related to the choice of the boundary conditions supercell-cluster approach, the resulting band-gap width, and the choice of the points to sample the Brillouin zone. The underestimated energy gap, resulting from the periodic conditions together with the local-density approximation to the exchange- correlation energy, leads to defect-related gap states that are strongly coupled to crystalline states within the center of the zone. This is shown to produce a strong effect even on relative energies. Our results indicate that in all E centers the donor atom occupies a nearly substitutional site, as opposed to the split-vacancy form adopted by the SnV complex in Si. The E centers can occur in four charge states, from positive to double negative, and produce occupancy levels at E0/+ = E v +0.1 eV, E-/0= E v +0.3 eV, and E=/-= E c -0.3 eV. DOI: 10.1103/PhysRevB.73.235213 PACS numbers: 61.72.Bb, 61.80.Az, 71.55.Cn, 71.70.Ej I. INTRODUCTION Intrinsic limitations in carrier mobility in Si, together with the recent advances in high-dielectrics research, has led to the resurgence of Ge as a key ingredient in a new generation of ultrafast devices to operate in a regime of tens of gigahertz. 1,2 Recent defect studies in Ge are scarce, particu- larly those dealing with the atomic and electronic details of elemental radiation induced defects. This deficiency applies not only to experimental reports see Refs. 3, 4, and refer- ences therein, but to modeling studies as well. 5–11 In this context, a detailed understanding of the properties of defects in Ge, especially those that may affect device yield and per- formance, is highly desirable. The class of vacancy-impurity complexes is particularly important as we know that many substitutional centers in- cluding dopantsmigrate by reacting with radiation- or ther- mally generated vacancies. 12 This also includes the actual Ge atoms in Ge crystals. According to 71 Ge tracer-diffusion measurements, self-diffusion in Ge is dominated by a va- cancy mechanism. 13,14 This is a major departure from what we know in Si, where self-interstitial mediated self-diffusion plays an important role. 15,16 The importance of vacancies in Ge has been recently highlighted after ab initio calculations predicting a formation energy for the single Ge vacancy as low as 1.7–1.9 eV depending on its charge state. 6 This is considerably less than the 3.55 eV formation energy of a self-interstitial in Ge, 17 and comparably less than that of a vacancy in Si which has been estimated as 4.4 eV. 18 It also suggests that at 600 ° C the concentration of thermal vacan- cies is about 10 12 cm -3 in Ge, contrasting with much less than one single vacancy per cm -3 under similar conditions in Si. Here, we report on ab initio density functional studies of a class of prominent radiation defects in Ge, namely donor- vacancy DVcomplexes D = P,As,Sb,Bi, also known as E centers, which are responsible for heavy compensation ef- fects in n-Ge crystals subject to MeV irradiation. We pay special attention to the electronic structure of such com- plexes, as well as to the approximations involved in treating the host crystal, i.e., by using Ge supercells or Ge clusters. Before summarizing previous experimental and theoreti- cal results concerning the E centers in Ge, it is instructive to present a short description of the analogous centers in Si. Early electron paramagnetic resonance EPRexperiments on e-irradiated n-doped Si established much of their proper- ties, including an atomic model shown in Fig. 1a. 19,20 This model is referred to as full-vacancy structure here, and we discern it from the split-vacancy model shown in Fig. 1b, which has been assigned to the tin-vacancy complex in Si. 21,22 The E centers in Si are produced by trapping mobile vacancies next to n-dopants. They introduce a deep acceptor state at around E c -0.4 eV, and are stable up to about 170 °C. 19,23 Three valence electrons from the group-V atom saturate Si atoms i', j ', and k', leaving two other elec- trons in a lone pair state below the valence band maximum. In the neutral defect, the Si radicals i, j , and k contribute with a total of three electrons. These hybridize to form a fully occupied a 1 ↑↓ state also lying below the valence band maxi- FIG. 1. Color onlineFull-vacancy aand split-vacancy b atomic models for a donor-vacancy complex in Si and Ge. The donor and host atoms are represented in blue and yellow, respec- tively. Vacant sites are shown in white. PHYSICAL REVIEW B 73, 235213 2006 1098-0121/2006/7323/23521310©2006 The American Physical Society 235213-1