Ground-state properties and high-pressure phase of beryllium chalcogenides BeSe, BeTe, and BeS A. Mun ˜ oz, P. Rodrı ´ guez-Herna ´ ndez, and A. Mujica Departamento de Fı ´sica Fundamental y Experimental, Facultad de Fı ´sica. Universidad de La Laguna, E-38204 La Laguna, Tenerife, Spain Received 22 April 1996 We present an ab initio pseudopotential study within the local density approximation of the ground-state and high-pressure phases of BeSe, BeTe, and BeS. We analyze the zinc-blende, NaCl, CsCl, NiAs, and -Sn structures. By calculating the total energy, atomic forces, and stress tensors we determine the structural parameters lattice constants, bulk moduli, etc.of these compounds and the transition pressure from the zinc-blende ( B 3 ) to the NiAs ( B 8) phase. The structural parameters and transition pressure for BeSe and BeTe compare quite well with recent experimental results. For BeS our results are predictions. S0163-18299604038-6 I. INTRODUCTION Little is known about beryllium chalcogenides BeS, BeSe, and BeTe. Recent experimental results 1 report the existence of a first-order transition between zinc-blende and NiAs phases in BeSe and BeTe at pressures of 61.36 GPa and 39.36 GPa, respectively. Among the IIA-VI compounds ex- perimentally investigated so far only for BeSe and BeTe has a first-order phase transition from the zinc-blende phase to the NiAs phase been reported; for the rest a phase transition between the NaCl and the CsCl structure has been observed 2 except for BeS where no experimental data are available. The beryllium compounds BeSe, BeTe, and BeS crystallize in the cubic zinc-blende structure. The rest of the chalco- genides of group IIA adopt the cubic NaCl structure except for BeO and MgTe, which have the wurtzite hexagonal structure. BeSe, BeTe, and BeS are particularly similar to the boron compounds BN, BP and BAs, having at ambient con- ditions the same crystal structure, wide band gap, and high bulk moduli. The zinc-blende compounds BN, BP, and BAs have an unusual behavior when compared to the other III-V compound families due to the small core size and the ab- sence of p electrons. Thus the study of the Be compound could help in the understanding of the behavior of the B compounds. In this work we concentrate our efforts in the theoretical study from ab initio pseudopotential theory of the structural phase transition of beryllium chalcogenides BeSe, BeTe, and BeS under pressure. We analyze the ground-state zinc- blende structure ZBand the sixfold coordinate cubic NaCl, the hexagonal NiAs, the cubic CsCl, and the tetragonal -Sn structures. The calculations are performed in the frame- work of the density functional theory with ab initio norm- conserving pseudopotential. 3 It is well known that this method is capable of giving accurate results for ground-state properties of a wide variety of semiconductors and metal materials. The ab initio pseudopotential method for total en- ergy calculations has been shown to be capable of predicting structural properties for group-IV elements 4,5 and III-V compounds. 6–8 Although the agreement between experiment and theory for group-IV elements is quite impressive, no- table discrepancies appear for some III-V compounds. Some difficulties arise from the fact that there is little experimental knowledge about the structure of the high-pressure phases and the incomplete theoretical study of these phases. The paper is organized as follows: In the next section we briefly describe the method of calculation and in Sec. III we present the study of the structural properties of the ground- state and high-pressure phases of BeSe, BeTe, and BeS. Fi- nally our conclusions are given in Sec. IV. II. METHOD We have used a first principles pseudopotential method within the local density approximation LDAformalism 3 to calculate the total energies of zinc-blende, NaCl, NiAs, CsCl, and -Sn phases for the beryllium compounds BeSe, BeTe, and BeS. The Ceperley-Alder form of the local den- sity approximation for the exchange correlation 9 was used. Norm-conserving nonlocal pseudopotentials were con- structed with the Kerker scheme. 10 We need to calculate small energy differences between phases. A basis set containing all plane waves up to the cutoff energy of 30 Ry was used for BeSe and BeTe which is sufficient to describe the energy difference between different phases with an accuracy of 1 meV/molecule; for BeS we need to increase the cutoff up to 90 Ry due to the hard potential of the sulfur atom. The Brillouin zone integrations were replaced by discrete k space summations. We use the standard k-points technique of Monkhorst and Pack. 11 In or- der to perform accurate Brillouin zone integrations for the semiconducting zinc-blende phase we use 28 k points and 168, 120, 110, and 100 k points for the Nias, CsCl, NaCl, and -Sn phases, respectively. The -Sn and NiAs structures have a single degree of freedom, which we take to be the c / a ratio. For these struc- tures we minimize the energy with respect to the internal degrees of freedom at each volume considered. For the hex- agonal NiAs structure we determine the two lattice constants a and c as follows. First we choose a unit cell volume V and PHYSICAL REVIEW B 1 NOVEMBER 1996-I VOLUME 54, NUMBER 17 54 0163-1829/96/5417/118614/$10.00 11 861 © 1996 The American Physical Society