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Title: Suppression of Superconductivity and Nematic Order in Fe1–ySe1–xSx (0 ≤ x ≤ 1; y ≤ 0.1) Crystals by Anion Height Disorder

Abstract

Connections between crystal chemistry and critical temperature Tc have been in the focus of superconductivity, one of the most widely studied phenomena in physics, chemistry and materials science alike. In most Fe-based superconductors materials chemistry and physics conspire so that Tc correlates with the average anion height above the Fe plane, i.e. with the geometry of the FeAs4 or FeCh4 (Ch = Te, Se, S) tetrahedron. Here, by synthesizing Fe1-ySe1-xSx (0 ≤ x ≤ 1, y ≤ 0.1) we find that in alloyed crystals Tc is not correlated with the anion height as most other Fe superconductors. Instead, changes in Tc(x) and tetragonal-to-orthorombic (nematic) transition Ts(x) on cooling are correlated with disorder in Fe vibrations in direction orthogonal to Fe planes, along the crystallographic c-axis. The disorder stems from the random nature of S substitution, causing deformed Fe(Se,S)4 tetrahedra with different Fe-Se and Fe-S bond distances. Our results provide evidence of Tc and Ts suppression by disorder in anion height. The connection to local crystal chemistry may be exploited in computational prediction of new superconducting materials with FeSe/S building blocks.

Authors:
ORCiD logo [1];  [2];  [3];  [2];  [4];  [5];  [3]; ORCiD logo [4]; ORCiD logo [2];  [6];  [5];  [7]; ORCiD logo [8]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Chongqing Univ. (China)
  2. Univ. of Belgrade (Serbia)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  4. Brookhaven National Lab. (BNL), Upton, NY (United States)
  5. Walther Meissner Institut, Garching (Germany); Technische Univ., Munich (Germany)
  6. Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II); ALBA Synchrotron Light Source, Cerdanyola del Valles (Spain)
  7. Univ. of Belgrade (Serbia); Serbian Academy of Sciences and Arts, Belgrade (Serbia)
  8. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Ministry of Education, Science and Technological Development of the Republic of Serbia; Science Fund of the Republic of Serbia
OSTI Identifier:
1897498
Report Number(s):
BNL-223672-2022-JAAM
Journal ID: ISSN 0020-1669; TRN: US2310799
Grant/Contract Number:  
SC0012704; 6062656
Resource Type:
Accepted Manuscript
Journal Name:
Inorganic Chemistry
Additional Journal Information:
Journal Volume: 61; Journal Issue: 29; Journal ID: ISSN 0020-1669
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Wang, Aifeng, Milosavljevic, Ana, Abeykoon, A. Milinda, Ivanovski, Valentin, Du, Qianheng, Baum, Andreas, Stavitski, Eli, Liu, Yu, Lazarevic, Nenad, Attenkofer, Klaus, Hackl, Rudi, Popovic, Zoran, and Petrovic, Cedomir. Suppression of Superconductivity and Nematic Order in Fe1–ySe1–xSx (0 ≤ x ≤ 1; y ≤ 0.1) Crystals by Anion Height Disorder. United States: N. p., 2022. Web. doi:10.1021/acs.inorgchem.2c00568.
Wang, Aifeng, Milosavljevic, Ana, Abeykoon, A. Milinda, Ivanovski, Valentin, Du, Qianheng, Baum, Andreas, Stavitski, Eli, Liu, Yu, Lazarevic, Nenad, Attenkofer, Klaus, Hackl, Rudi, Popovic, Zoran, & Petrovic, Cedomir. Suppression of Superconductivity and Nematic Order in Fe1–ySe1–xSx (0 ≤ x ≤ 1; y ≤ 0.1) Crystals by Anion Height Disorder. United States. https://doi.org/10.1021/acs.inorgchem.2c00568
Wang, Aifeng, Milosavljevic, Ana, Abeykoon, A. Milinda, Ivanovski, Valentin, Du, Qianheng, Baum, Andreas, Stavitski, Eli, Liu, Yu, Lazarevic, Nenad, Attenkofer, Klaus, Hackl, Rudi, Popovic, Zoran, and Petrovic, Cedomir. Wed . "Suppression of Superconductivity and Nematic Order in Fe1–ySe1–xSx (0 ≤ x ≤ 1; y ≤ 0.1) Crystals by Anion Height Disorder". United States. https://doi.org/10.1021/acs.inorgchem.2c00568. https://www.osti.gov/servlets/purl/1897498.
@article{osti_1897498,
title = {Suppression of Superconductivity and Nematic Order in Fe1–ySe1–xSx (0 ≤ x ≤ 1; y ≤ 0.1) Crystals by Anion Height Disorder},
author = {Wang, Aifeng and Milosavljevic, Ana and Abeykoon, A. Milinda and Ivanovski, Valentin and Du, Qianheng and Baum, Andreas and Stavitski, Eli and Liu, Yu and Lazarevic, Nenad and Attenkofer, Klaus and Hackl, Rudi and Popovic, Zoran and Petrovic, Cedomir},
abstractNote = {Connections between crystal chemistry and critical temperature Tc have been in the focus of superconductivity, one of the most widely studied phenomena in physics, chemistry and materials science alike. In most Fe-based superconductors materials chemistry and physics conspire so that Tc correlates with the average anion height above the Fe plane, i.e. with the geometry of the FeAs4 or FeCh4 (Ch = Te, Se, S) tetrahedron. Here, by synthesizing Fe1-ySe1-xSx (0 ≤ x ≤ 1, y ≤ 0.1) we find that in alloyed crystals Tc is not correlated with the anion height as most other Fe superconductors. Instead, changes in Tc(x) and tetragonal-to-orthorombic (nematic) transition Ts(x) on cooling are correlated with disorder in Fe vibrations in direction orthogonal to Fe planes, along the crystallographic c-axis. The disorder stems from the random nature of S substitution, causing deformed Fe(Se,S)4 tetrahedra with different Fe-Se and Fe-S bond distances. Our results provide evidence of Tc and Ts suppression by disorder in anion height. The connection to local crystal chemistry may be exploited in computational prediction of new superconducting materials with FeSe/S building blocks.},
doi = {10.1021/acs.inorgchem.2c00568},
journal = {Inorganic Chemistry},
number = 29,
volume = 61,
place = {United States},
year = {Wed Jul 13 00:00:00 EDT 2022},
month = {Wed Jul 13 00:00:00 EDT 2022}
}

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