Correlated electronic structure and optical response of rare-earth based semiconductors
(2021) In Physical Review B 103(24).- Abstract
The coexistence of Mott localized f states with wide conduction and valence bands in f-electron semiconductors results, quite generically, in a complex optical response with the nature of the absorption edge difficult to resolve both experimentally and theoretically. Here, we combine a dynamical mean-field theory approach to localized 4f shells with an improved description of band gaps by a semilocal exchange-correlation potential to calculate the optical properties of the light rare-earth fluorosulfides LnSF (Ln=Pr, Nd, Sm, Gd) from first principles. In agreement with experiment, we find the absorption edge in SmSF to stem from S-3p to Sm-4f transitions, while the Gd compound behaves as an ordinary p-d gap semiconductor. In the... (More)
The coexistence of Mott localized f states with wide conduction and valence bands in f-electron semiconductors results, quite generically, in a complex optical response with the nature of the absorption edge difficult to resolve both experimentally and theoretically. Here, we combine a dynamical mean-field theory approach to localized 4f shells with an improved description of band gaps by a semilocal exchange-correlation potential to calculate the optical properties of the light rare-earth fluorosulfides LnSF (Ln=Pr, Nd, Sm, Gd) from first principles. In agreement with experiment, we find the absorption edge in SmSF to stem from S-3p to Sm-4f transitions, while the Gd compound behaves as an ordinary p-d gap semiconductor. In the unexplored PrSF and NdSF systems we predict a rather unique occurrence of strongly hybridized 4f-5d states at the bottom of the conduction band. The nature of the absorption edge results in a characteristic anisotropy of the optical conductivity in each system, which may be used as a fingerprint of the relative energetic positions of different states.
(Less)
- author
- Galler, Anna ; Boust, James ; Demourgues, Alain ; Biermann, Silke LU and Pourovskii, Leonid V.
- organization
- publishing date
- 2021
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Physical Review B
- volume
- 103
- issue
- 24
- article number
- L241105
- publisher
- American Physical Society
- external identifiers
-
- scopus:85108101039
- ISSN
- 2469-9950
- DOI
- 10.1103/PhysRevB.103.L241105
- language
- English
- LU publication?
- yes
- id
- 42e1f5ea-d724-47d7-883f-e18368086128
- date added to LUP
- 2021-07-15 13:42:32
- date last changed
- 2022-04-27 02:47:34
@article{42e1f5ea-d724-47d7-883f-e18368086128,
abstract = {{<p>The coexistence of Mott localized f states with wide conduction and valence bands in f-electron semiconductors results, quite generically, in a complex optical response with the nature of the absorption edge difficult to resolve both experimentally and theoretically. Here, we combine a dynamical mean-field theory approach to localized 4f shells with an improved description of band gaps by a semilocal exchange-correlation potential to calculate the optical properties of the light rare-earth fluorosulfides LnSF (Ln=Pr, Nd, Sm, Gd) from first principles. In agreement with experiment, we find the absorption edge in SmSF to stem from S-3p to Sm-4f transitions, while the Gd compound behaves as an ordinary p-d gap semiconductor. In the unexplored PrSF and NdSF systems we predict a rather unique occurrence of strongly hybridized 4f-5d states at the bottom of the conduction band. The nature of the absorption edge results in a characteristic anisotropy of the optical conductivity in each system, which may be used as a fingerprint of the relative energetic positions of different states.</p>}},
author = {{Galler, Anna and Boust, James and Demourgues, Alain and Biermann, Silke and Pourovskii, Leonid V.}},
issn = {{2469-9950}},
language = {{eng}},
number = {{24}},
publisher = {{American Physical Society}},
series = {{Physical Review B}},
title = {{Correlated electronic structure and optical response of rare-earth based semiconductors}},
url = {{http://dx.doi.org/10.1103/PhysRevB.103.L241105}},
doi = {{10.1103/PhysRevB.103.L241105}},
volume = {{103}},
year = {{2021}},
}