Ge-based Clinopyroxene series: first principles and experimental local probe study

Fuente: arXiv
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Main Authors: Moreira, Ricardo P., da Silva, E. Lora, Oliveira, Gonçalo N. P., Rocha-Rodrigues, Pedro, Stroppa, Alessandro, Colin, Claire V., Darie, Céline, Correia, João G., Assali, Lucy V. C., Petrilli, Helena M., Lopes, Armandina M. L., Araújo, João P.
Format: Preprint
Published: 2024
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author Moreira, Ricardo P.
da Silva, E. Lora
Oliveira, Gonçalo N. P.
Rocha-Rodrigues, Pedro
Stroppa, Alessandro
Colin, Claire V.
Darie, Céline
Correia, João G.
Assali, Lucy V. C.
Petrilli, Helena M.
Lopes, Armandina M. L.
Araújo, João P.
author_facet Moreira, Ricardo P.
da Silva, E. Lora
Oliveira, Gonçalo N. P.
Rocha-Rodrigues, Pedro
Stroppa, Alessandro
Colin, Claire V.
Darie, Céline
Correia, João G.
Assali, Lucy V. C.
Petrilli, Helena M.
Lopes, Armandina M. L.
Araújo, João P.
contents The structural and electronic properties of the CaMnGe$_2$O$_6$ and SrMnGe$_2$O$_6$ clinopyroxene systems have been investigated by means of perturbed angular correlation (PAC) measurements, performed at ISOLDE, combined with $ab-initio$ electronic structure calculations within the density functional theory (DFT) framework. The partial density of states (PDOS) of the CaMnGe$_2$O$_6$ and SrMnGe$_2$O$_6$ stable compounds has been determined, and it has been observed that the requirement of including an on-site Hubbard-$U$ potential was necessary in order to describe the highly correlated Mn $3d$-states. By considering $U_{eff}$=4 eV, we obtained a band gap width of 1.82 eV and 1.70 eV, for the CaMnGe$_2$O$_6$ and SrMnGe$_2$O$_6$, respectively. Combining electric field gradient (EFG) first principles calculations, using a supercell scheme, with experimental PAC results, we were able to infer that the Cd probe can replace either the $A$ (Ca, Sr) or the Mn sites in the crystalline structures. We also showed that Cd substitution is expected to lead to a reduction in the width of the band gap in these systems, evidencing opportunities for potential band-gap engineering.
format Preprint
id arxiv_https___arxiv_org_abs_2407_21749
institution arXiv
publishDate 2024
record_format arxiv
spellingShingle Ge-based Clinopyroxene series: first principles and experimental local probe study
Moreira, Ricardo P.
da Silva, E. Lora
Oliveira, Gonçalo N. P.
Rocha-Rodrigues, Pedro
Stroppa, Alessandro
Colin, Claire V.
Darie, Céline
Correia, João G.
Assali, Lucy V. C.
Petrilli, Helena M.
Lopes, Armandina M. L.
Araújo, João P.
Materials Science
Strongly Correlated Electrons
The structural and electronic properties of the CaMnGe$_2$O$_6$ and SrMnGe$_2$O$_6$ clinopyroxene systems have been investigated by means of perturbed angular correlation (PAC) measurements, performed at ISOLDE, combined with $ab-initio$ electronic structure calculations within the density functional theory (DFT) framework. The partial density of states (PDOS) of the CaMnGe$_2$O$_6$ and SrMnGe$_2$O$_6$ stable compounds has been determined, and it has been observed that the requirement of including an on-site Hubbard-$U$ potential was necessary in order to describe the highly correlated Mn $3d$-states. By considering $U_{eff}$=4 eV, we obtained a band gap width of 1.82 eV and 1.70 eV, for the CaMnGe$_2$O$_6$ and SrMnGe$_2$O$_6$, respectively. Combining electric field gradient (EFG) first principles calculations, using a supercell scheme, with experimental PAC results, we were able to infer that the Cd probe can replace either the $A$ (Ca, Sr) or the Mn sites in the crystalline structures. We also showed that Cd substitution is expected to lead to a reduction in the width of the band gap in these systems, evidencing opportunities for potential band-gap engineering.
title Ge-based Clinopyroxene series: first principles and experimental local probe study
topic Materials Science
Strongly Correlated Electrons
url https://arxiv.org/abs/2407.21749