Global and local structures of the Ge-Sb-Te ternary alloy system for a phase-change memory device Jae-Hyeon Eom, 1 Young-Gui Yoon, 2 Changwon Park, 1 Hoonkyung Lee, 1 Jino Im, 1 Dong-Seok Suh, 3 Jin-Seo Noh, 3 Yoonho Khang, 3 and Jisoon Ihm 1 1 School of Physics, Seoul National University, Seoul 151-747, Korea 2 Department of Physics, Chung-Ang University, Seoul, Korea 3 Materials Center, Samsung Advanced Institute of Technology, Mt. 14-1, Nongseo-Ri, Giheung-Eup, Yongin-Si, Gyeonggi-Do, 449-712, Korea Received 14 October 2005; revised manuscript received 27 March 2006; published 6 June 2006 A detailed theoretical investigation on the global and local structures of the Ge-Sb-TeGSTternary alloy system for the phase-change memory is presented. We examine the cohesive energy of the GeTe n Sb 2 Te 3 m homologous series as well as the dependence of the energy on the atomic distribution. We show that the cohesive energy decreases with increasing vacancy concentration and the vacancies repel each other to mini- mize the number of dangling bonds. In Ge 2 Sb 2 Te 5 , Sb and Ge atoms favor two-dimensional layeredand three-dimensional agglomeratedarrangements, respectively. In Ge 1 Sb 2 Te 4 , on the other hand, Ge atoms tend to form a two-dimensional layered structure. Possible structural building blocks of the GST system are pro- posed based on the density-functional theory total energy calculations. DOI: 10.1103/PhysRevB.73.214202 PACS numbers: 71.15.Nc, 77.84.Bw I. INTRODUCTION Recently, the rapid growth of the multimedia technology has demanded fast and small rewritable nonvolatile memo- ryNVMdevices as essential components. Various concepts for the next-generation NVM have been proposed so far. 1 Among the candidates, the phase-change memoryPCMuti- lizes the resistivity difference between crystalline and amor- phous phases. 2 It is noted that a typical resistivity ratio be- tween the amorphous and the crystalline phase is more than 1000. 3,4 This huge difference in resistivity establishes the PCM as a strong candidate for the next-generation NVM. For the PCM, stable amorphous and crystalline phases real- izable in a single material are required. Ge-Sb-Te GSTter- nary alloys are so far known as the best for the PCM due to their stability 10 yearsand the fast switching time 100 ns. The GST is already used for rewritable compact disks and digital video disks, taking advantage of the differ- ence in reflectivity between two phases. However, knowl- edge of the structure and basic physical properties of the GST is still primitive, and the fact that the GST is a ternary alloy makes the experimental and theoretical analysis very difficult. Admitting that the GST has a complex composition and structure, some experimental data still exist which can guide us into a partial understanding of the system. First, the phase transition between the crystalline and amorphous phase is very fast and reversible, which implies that the structure of the amorphous phase may not be totally different from that of the crystal. Therefore, the crystalline phase of the GST could presumably provide some essential information on the amorphous phase. The GST is known to show two kinds of crystal structures; namely, the rocksaltNaCl-like and hexagonal. 3,5,6 When the amorphous GST is heated, transi- tion to the rocksalt-like structure occurs around 400 K, and subsequent transition to the hexagonal structure around 500 K. The hexagonal structure is stable at low temperature 6 and the rocksalt-like structure is a metastable phase. In prac- tice, only the metastable phases occurs in fast transition to the crystalline phase. Since the phase transition between the rocksalt-like metastable and the amorphous phase is used in the operation of the PCM, we will now concentrate on the metastable rocksalt-like structure. X-ray diffraction study shows that 4asites constituting one of the two sublattices of the NaCl structure are fully occupied by Te, and 4bsites are occupied by Ge, Sb, and the vacancy. Second, GST ternary systems are composed of GeTe and Sb 2 Te 3 binary alloys. This means that composition of the GST system is given by GeTe n Sb 2 Te 3 m with inte- gers n and m. Moreover, a recent study on the phonon mode of the GST system indicates that there is a local order in units of GeTe and Sb 2 Te 3 . 7 We may expect that the distribu- tion of Ge and Sb atoms, and vacancies on 4bsites are not completely random, and the metastable phase of the GST system is a somewhat distortedrocksalt structure maintain- ing some local order of the structural subunits of GeTe and Sb 2 Te 3 . It is noted that recent studies on the local structure of the GST show that the crystal structure is distorted, and there exist long and short bonds. 8–10 A building block of the Ge 2 Sb 2 Te 5 unit has been proposed in the literature based on the extended x-ray absorption fine structure data. 8 However, their model is two-dimensional and does not include the structure of the subunits GeTe and Sb 2 Te 3 ; a more realistic structure of the GST with a three-dimensional building block originating from GeTe and Sb 2 Te 3 is desirable. In this work, we calculate the cohesive energy of the GeTe n Sb 2 Te 3 m homologous series. We also investigate the dependence of the energy on the distribution of the Ge and Sb atoms and vacancies for Ge 2 Sb 2 Te 5 and Ge 1 Sb 2 Te 4 , and propose a possible local structure based on the ab initio supercell electronic structure calculations. II. COMPUTATIONAL METHODS Electronic structure calculations were performed using the self-consistent ab initio pseudo-potential method with the PHYSICAL REVIEW B 73, 214202 2006 1098-0121/2006/7321/2142025©2006 The American Physical Society 214202-1