Investigating charge carrier scattering processes in anisotropic semiconductors through first-principles calculations: the case of p-type SnSe

Author(s)

Chaves, Anderson S. ^[1] ; Gonzalez-Romero, Robert Luis ^[2] ; Melendez, Juan J. ^{[3, 4]} ; Antonelli, Alex ^{[1, 5]}

Affiliation

^[1] Univ Estadual Campinas, Inst Fis Gleb Wataghin, UNICAMP, BR-13083859 Campinas, SP - Brazil

^[2] Univ Pablo de Olavide, Dept Sistemas Fis Quim & Nat, Ctra Utrera, Km 1, Seville 41013 - Spain

^[3] Univ Extremadura, Dept Phys, Ave Elvas S-N, Badajoz 06006 - Spain

^[4] Inst Adv Sci Comp Extremadura ICCAEx, Avda Elvas S-N, Badajoz 06006 - Spain

^[5] Univ Estadual Campinas, Ctr Computat Engn & Sci, UNICAMP, BR-13083859 Campinas, SP - Brazil

• Document type: Journal article
• Source: Physical Chemistry Chemical Physics; v. 23, n. 2, p. 900-913, JAN 14 2021.
• Web of Science Citations: 0

Abstract

Efficient ab initio computational methods for the calculation of the thermoelectric transport properties of materials are of great interest for energy harvesting technologies. The constant relaxation time approximation (CRTA) has been largely used to efficiently calculate thermoelectric coefficients. However, CRTA usually does not hold for real materials. Here we go beyond the CRTA by incorporating realistic k-dependent relaxation time models of the temperature dependence of the main scattering processes, namely, screened polar and nonpolar scattering by optical phonons, scattering by acoustic phonons, and scattering by ionized impurities with screening. Our relaxation time models are based on a smooth Fourier interpolation of Kohn-Sham eigenvalues and its derivatives, taking into account non-parabolicity (beyond the parabolic or Kane models), degeneracy and multiplicity of the energy bands on the same footing, within very low computational cost. In order to test our methodology, we calculated the anisotropic thermoelectric transport properties of the low temperature phase (Pnma) of intrinsic p-type and hole-doped tin selenide (SnSe). Our results are in quantitative agreement with experimental data, regarding the evolution of the anisotropic thermoelectric coefficients with both temperature and chemical potential. Hence, from this picture, we also obtained the evolution and understanding of the main scattering processes of the overall thermoelectric transport in p-type SnSe. (AU)

• FAPESP's process: 15/26434-2 - Study of the electronic, structural, and transport properties of materials for thermoelectric applications via ab initio calculations
• Grantee: Anderson Silva Chaves
• Support Opportunities: Scholarships in Brazil - Post-Doctorate
• FAPESP's process: 16/23891-6 - Computer modeling of condensed matter
• Grantee: Alex Antonelli
• Support Opportunities: Research Projects - Thematic Grants
• FAPESP's process: 17/26105-4 - Multi-user equipment approved in grant 2016/23891-6 high performace computational cluster
• Grantee: Alex Antonelli
• Support Opportunities: Multi-user Equipment Program
• FAPESP's process: 13/08293-7 - CCES - Center for Computational Engineering and Sciences
• Grantee: Munir Salomao Skaf
• Support Opportunities: Research Grants - Research, Innovation and Dissemination Centers - RIDC
• FAPESP's process: 19/26088-8 - Study of doping effects in As2Se3 and As2S3 from first-principles calculations
• Grantee: Anderson Silva Chaves
• Support Opportunities: Scholarships in Brazil - Post-Doctorate
• FAPESP's process: 10/16970-0 - Computational modeling of condensed matter: a multiscale approach
• Grantee: Alex Antonelli
• Support Opportunities: Research Projects - Thematic Grants