First-principles study of the lattice dynamics of Sb2S3
We present a lattice dynamics study of orthorhombic antimony sulphide (Sb2S3) obtained using density-functional calculations in conjunction with the supercell force-constant method. The effect of Born effective charges is taken into account using a mixed-space approach, resulting in the splitting of...
| Main Authors: | , , , |
|---|---|
| Other Authors: | |
| Format: | Journal Article |
| Language: | English |
| Published: |
2014
|
| Subjects: | |
| Online Access: | https://hdl.handle.net/10356/105179 http://hdl.handle.net/10220/20435 |
| _version_ | 1824454925452574720 |
|---|---|
| author | Liu, Yun Eddie Chua, Kun Ting Sum, Tze Chien Gan, Chee Kwan |
| author2 | School of Physical and Mathematical Sciences |
| author_facet | School of Physical and Mathematical Sciences Liu, Yun Eddie Chua, Kun Ting Sum, Tze Chien Gan, Chee Kwan |
| author_sort | Liu, Yun |
| collection | NTU |
| description | We present a lattice dynamics study of orthorhombic antimony sulphide (Sb2S3) obtained using density-functional calculations in conjunction with the supercell force-constant method. The effect of Born effective charges is taken into account using a mixed-space approach, resulting in the splitting of longitudinal and transverse optical (LO-TO) phonon branches near the zone center. Zone-center frequencies agree well with Raman scattering experiments. Due to the slow decay of the interatomic force constants (IFC), a minimal 2 × 4 × 2 supercell (Pnma setting) with 320 atoms is crucial for an accurate determination of the dispersion relations. Smaller supercells result in artificial acoustic phonon softening and unphysical lifting of degeneracies along high symmetry directions. We propose a scheme to investigate the convergence of the IFC with respect to the supercell sizes. The phonon softening can be attributed to the periodic images that affect the accuracy of the force constants, and the truncation of long-ranged forces. The commensuration of the q-vectors with the supercell size is crucial to preserve degeneracies in Sb2S3 crystals. |
| first_indexed | 2025-02-19T03:30:03Z |
| format | Journal Article |
| id | ntu-10356/105179 |
| institution | Nanyang Technological University |
| language | English |
| last_indexed | 2025-02-19T03:30:03Z |
| publishDate | 2014 |
| record_format | dspace |
| spelling | ntu-10356/1051792023-02-28T19:45:37Z First-principles study of the lattice dynamics of Sb2S3 Liu, Yun Eddie Chua, Kun Ting Sum, Tze Chien Gan, Chee Kwan School of Physical and Mathematical Sciences DRNTU::Science::Physics DRNTU::Science::Chemistry We present a lattice dynamics study of orthorhombic antimony sulphide (Sb2S3) obtained using density-functional calculations in conjunction with the supercell force-constant method. The effect of Born effective charges is taken into account using a mixed-space approach, resulting in the splitting of longitudinal and transverse optical (LO-TO) phonon branches near the zone center. Zone-center frequencies agree well with Raman scattering experiments. Due to the slow decay of the interatomic force constants (IFC), a minimal 2 × 4 × 2 supercell (Pnma setting) with 320 atoms is crucial for an accurate determination of the dispersion relations. Smaller supercells result in artificial acoustic phonon softening and unphysical lifting of degeneracies along high symmetry directions. We propose a scheme to investigate the convergence of the IFC with respect to the supercell sizes. The phonon softening can be attributed to the periodic images that affect the accuracy of the force constants, and the truncation of long-ranged forces. The commensuration of the q-vectors with the supercell size is crucial to preserve degeneracies in Sb2S3 crystals. Accepted version 2014-09-01T01:17:20Z 2019-12-06T21:47:12Z 2014-09-01T01:17:20Z 2019-12-06T21:47:12Z 2013 2013 Journal Article Liu, Y., Eddie Chua, K. T., Sum, T. C., & Gan, C. K. (2013). First-principles study of the lattice dynamics of Sb2S3. Physical Chemistry Chemical Physics, 16(1), 345-350. https://hdl.handle.net/10356/105179 http://hdl.handle.net/10220/20435 10.1039/c3cp53879f en Physical chemistry chemical physics © 2014 Royal Society of Chemistry. This is the author created version of a work that has been peer reviewed and accepted for publication by Physical Chemistry Chemical Physics, Royal Society of Chemistry. It incorporates referee’s comments but changes resulting from the publishing process, such as copyediting, structural formatting, may not be reflected in this document. The published version is available at: [http://dx.doi.org/10.1039/C3CP53879F]. application/pdf |
| spellingShingle | DRNTU::Science::Physics DRNTU::Science::Chemistry Liu, Yun Eddie Chua, Kun Ting Sum, Tze Chien Gan, Chee Kwan First-principles study of the lattice dynamics of Sb2S3 |
| title | First-principles study of the lattice dynamics of Sb2S3 |
| title_full | First-principles study of the lattice dynamics of Sb2S3 |
| title_fullStr | First-principles study of the lattice dynamics of Sb2S3 |
| title_full_unstemmed | First-principles study of the lattice dynamics of Sb2S3 |
| title_short | First-principles study of the lattice dynamics of Sb2S3 |
| title_sort | first principles study of the lattice dynamics of sb2s3 |
| topic | DRNTU::Science::Physics DRNTU::Science::Chemistry |
| url | https://hdl.handle.net/10356/105179 http://hdl.handle.net/10220/20435 |
| work_keys_str_mv | AT liuyun firstprinciplesstudyofthelatticedynamicsofsb2s3 AT eddiechuakunting firstprinciplesstudyofthelatticedynamicsofsb2s3 AT sumtzechien firstprinciplesstudyofthelatticedynamicsofsb2s3 AT gancheekwan firstprinciplesstudyofthelatticedynamicsofsb2s3 |