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Title: Glass-Like Through-Plane Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La 0.5Sr 0.5CoO 3– δ [Glass-Like Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La 0.5Sr 0.5CoO 3– δ]

Here, ultrafast time-domain thermoreflectance (TDTR) is utilized to extract the through-plane thermal conductivity (Λ LSCO) of epitaxial La 0.5Sr 0.5CoO 3–δ (LSCO) of varying thickness (<20 nm) on LaAlO 3 and SrTiO 3 substrates. These LSCO films possess ordered oxygen vacancies as the primary means of lattice mismatch accommodation with the substrate, which induces compressive/tensile strain and thus controls the orientation of the oxygen vacancy ordering (OVO). TDTR results demonstrate that the room-temperature Λ LSCO of LSCO on both substrates (1.7 W m –1 K –1) are nearly a factor of four lower than that of bulk single-crystal LSCO (6.2 W m –1 K –1). Remarkably, this approaches the lower limit of amorphous oxides (e.g., 1.3 W m –1 K –1 for glass), with no dependence on the OVO orientation. Through theoretical simulations, origins of the glass-like thermal conductivity of LSCO are revealed as a combined effect resulting from oxygen vacancies (the dominant factor), Sr substitution, size effects, and the weak electron/phonon coupling within the LSCO film. The absence of OVO dependence in the measured Λ LSCO is rationalized by two main effects: (1) the nearly isotropic phononic thermal conductivity resulting from the imperfect OVO planes when δ is small;more » (2) the missing electronic contribution to Λ LSCO along the through-plane direction for these ultrathin LSCO films on insulating substrates.« less
Authors:
 [1] ;  [1] ;  [2] ;  [1] ;  [3] ;  [3] ;  [4] ;  [4] ;  [2] ;  [1] ;  [1]
  1. Univ. of Minnesota, Minneapolis, MN (United States)
  2. Purdue Univ., West Lafayette, IN (United States)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Univ. Complutense de Madrid, Madrid (Spain)
Publication Date:
Grant/Contract Number:
AC02-06CH11357; FG02-06ER46275; SC0016371
Type:
Accepted Manuscript
Journal Name:
Advanced Functional Materials
Additional Journal Information:
Journal Volume: 27; Journal Issue: 47; Journal ID: ISSN 1616-301X
Publisher:
Wiley
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
National Natural Science Foundation of China (NNSFC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; National Science Foundation (NSF); Spanish Ministerio de Economia y Competitividad (MINECO); USDOE
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Boltzmann transport equation; LSCO; TDTR; molecular dynamics simulation; nanoscale epitaxial LSCO; oxygen vacancies; perovskite; thermal conductivity; time-domain thermoreflectance
OSTI Identifier:
1415607
Alternate Identifier(s):
OSTI ID: 1407813

Wu, Xuewang, Walter, Jeff, Feng, Tianli, Zhu, Jie, Zheng, Hong, Mitchell, John F., Biskup, Neven, Varela, Maria, Ruan, Xiulin, Leighton, Chris, and Wang, Xiaojia. Glass-Like Through-Plane Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ [Glass-Like Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ]. United States: N. p., Web. doi:10.1002/adfm.201704233.
Wu, Xuewang, Walter, Jeff, Feng, Tianli, Zhu, Jie, Zheng, Hong, Mitchell, John F., Biskup, Neven, Varela, Maria, Ruan, Xiulin, Leighton, Chris, & Wang, Xiaojia. Glass-Like Through-Plane Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ [Glass-Like Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ]. United States. doi:10.1002/adfm.201704233.
Wu, Xuewang, Walter, Jeff, Feng, Tianli, Zhu, Jie, Zheng, Hong, Mitchell, John F., Biskup, Neven, Varela, Maria, Ruan, Xiulin, Leighton, Chris, and Wang, Xiaojia. 2017. "Glass-Like Through-Plane Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ [Glass-Like Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ]". United States. doi:10.1002/adfm.201704233. https://www.osti.gov/servlets/purl/1415607.
@article{osti_1415607,
title = {Glass-Like Through-Plane Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ [Glass-Like Thermal Conductivity Induced by Oxygen Vacancies in Nanoscale Epitaxial La0.5Sr0.5CoO3–δ]},
author = {Wu, Xuewang and Walter, Jeff and Feng, Tianli and Zhu, Jie and Zheng, Hong and Mitchell, John F. and Biskup, Neven and Varela, Maria and Ruan, Xiulin and Leighton, Chris and Wang, Xiaojia},
abstractNote = {Here, ultrafast time-domain thermoreflectance (TDTR) is utilized to extract the through-plane thermal conductivity (ΛLSCO) of epitaxial La0.5Sr0.5CoO3–δ (LSCO) of varying thickness (<20 nm) on LaAlO3 and SrTiO3 substrates. These LSCO films possess ordered oxygen vacancies as the primary means of lattice mismatch accommodation with the substrate, which induces compressive/tensile strain and thus controls the orientation of the oxygen vacancy ordering (OVO). TDTR results demonstrate that the room-temperature ΛLSCO of LSCO on both substrates (1.7 W m–1 K–1) are nearly a factor of four lower than that of bulk single-crystal LSCO (6.2 W m–1 K–1). Remarkably, this approaches the lower limit of amorphous oxides (e.g., 1.3 W m–1 K–1 for glass), with no dependence on the OVO orientation. Through theoretical simulations, origins of the glass-like thermal conductivity of LSCO are revealed as a combined effect resulting from oxygen vacancies (the dominant factor), Sr substitution, size effects, and the weak electron/phonon coupling within the LSCO film. The absence of OVO dependence in the measured ΛLSCO is rationalized by two main effects: (1) the nearly isotropic phononic thermal conductivity resulting from the imperfect OVO planes when δ is small; (2) the missing electronic contribution to ΛLSCO along the through-plane direction for these ultrathin LSCO films on insulating substrates.},
doi = {10.1002/adfm.201704233},
journal = {Advanced Functional Materials},
number = 47,
volume = 27,
place = {United States},
year = {2017},
month = {11}
}

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