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SCIENCE CHINA Materials, Volume 63 , Issue 9 : 1750-1758(2020) https://doi.org/10.1007/s40843-020-1344-x

High-pressure synthesis, crystal structure and physical properties of a new Cr-based arsenide La3CrAs5

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  • ReceivedJan 14, 2020
  • AcceptedApr 11, 2020
  • PublishedJun 3, 2020

Abstract

In La-Cr-As system, the first ternary compound La3CrAs5 has been successfully synthesized under high-pressure and high-temperature conditions. La3CrAs5 crystallizes into a hexagonal Hf5Sn3Cu-anti type structure with a space group of P63/mcm (No. 193) and lattice parameters of a=b=8.9845 Å and c=5.8897 Å. The structure contains face-sharing octahedral CrAs6 chains along the c-axis, which are arranged triangularly in the ab-plane and separated by a significantly large distance of 8.9845 Å. The magnetic properties, resistivity and specific heat measurements were performed. La3CrAs5 exhibits a metallic state with Fermi liquid behavior at low temperatures and undergoes a ferromagnetic transition at Curie temperature TC ~50 K. First-principles theoretical studies were conducted to calculate its band structure and density of states (DOS), which indicated that the non-negligible contribution of La to the DOS near the Fermi level caused La3CrAs5 to be a three-dimensional (3D) metal. The crystal orbital Hamilton population (−COHP) was also calculated to explain the global stability and bonding characteristics in the structure of La3CrAs5.


Funded by

the National Key R&D Program of China and the National Natural Science Foundation of China(2018YFA0305700,11974410,2017YFA0302900,2015CB92130011534016,11974062)


Acknowledgment

This work was supported by the National Key R&D Program of China and the National Natural Science Foundation of China (2018YFA0305700, 11974410, 2017YFA0302900, 2015CB921300, 11534016 and 11974062).


Interest statement

The authors declare that they have no conflict of interest.


Contributions statement

Jin C and Wang X conceived and supervised this project. Duan L preformed most of experiments including the synthesis, characterizations and physical properties measurement with the assistance of Zhang J, Li W, Zhao J, Cao L, Deng Z and Yu R. Hu Z, Lin HJ, and Chen CT performed the XAS measurements and data analysis. The calculations were carried out by Zhan F and Wang R. Duan L, Wang X and Jin C wrote the paper in discussion with other co-authors.


Author information

Lei Duan is currently a PhD candidate at the Institute of Physics, Chinese Academy of Sciences (IOPCAS). He received his BSc degree (majored in physics) from Jilin University, China in 2010. His PhD research focuses on using high-pressure technique to explore and synthesize new quantum materials such as superconductors and quasi one-dimensional (1D) materials.


Xiancheng Wang is currently an associate professor at the IOPCAS. He received his PhD degree from Jilin University in 2005, and then became a postdoctoral fellow in Tsinghua University. Since 2008, he has worked at IOPCAS. His research interests include exploring new materials especially using high pressure technique and studying their novel physics, such as superconductors and the materials with quasi one-dimensional (1D) spin chains or 1D conducting chains.


Rui Wang received his PhD degree in condensed matter physics from Chongqing University (CQU), China in 2012. He then worked as a faculty in CQU. In 2017–2018, he came to Southern University of Science and Technology as a senior visiting scholar. Currently, he is an associate professor in the Department of Physics, CQU. His research interests include computational condensed matter physics, design of topological insulators and semimetals, and defect physics.


Changqing Jin received his PhD degree at the IOPCAS in 1991. He was an associate professor (1996), and is currently a professor (1998) at the IOPCAS. He is team leader of IOPCAS on studies of new emergent materials by design especially via developing synergetic high-pressure extreme conditions.


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  • Figure 1

    The PXRD pattern of La3CrAs5 and the refinement with the space group of P63/mcm (No. 193).

  • Figure 2

    (a) The crystal structure of La3CrAs5 with the projection along the c axis, showing the triangular lattice form and chain structure characteristic. (b) The sketch of CrAs6 octahedron chain in La3CrAs5. (c) The partial structure of La3CrAs5, displaying the bridge of LaAs9 polyhedron between CrAs6 octahedral chains and As2 chains.

  • Figure 3

    The calculated electronic band structures along high symmetry paths where the spin up and spin down bands are denoted by red and blue lines (right panel) and the spin-resolved partial density of states (left panel).

  • Figure 4

    −COHP plot for the selected interactions.

  • Figure 5

    Cr-L2,3 XAS of La3CrAs5 with that of Cr2O3 as Cr3+ reference.

  • Figure 6

    (a) Temperature dependence of magnetic susceptibility χ(T) (left axis) and inverse magnetization χ−1(T) (right axis) for La3CrAs5. The purple line is the fit of Curie-Weiss law between 150 and 300 K. The inset shows dχ/dT vs. T. (b) The magnetic hysteresis curve measured at 2 and 100 K. The inset presents the enlarged view of the low-field data at 2 K.

  • Figure 7

    (a) Temperature dependence of resistivity of La3CrAs5. The left inset shows the temperature dependence of dρ/dT; The right inset shows the T2 variation of ρ at low temperature (2–45 K). (b) Temperature-dependent heat capacity between 2 and 100 K for La3CrAs5. The inset displays the fitting results of heat capacity at low temperature.

  • Table 1   The summary of the crystallographic data at room temperature for La3CrAs5a

    Site

    Wyck.

    x

    y

    z

    U (Å)

    La

    6g

    0.6227(7)

    0

    1/4

    0.0122

    Cr

    2b

    0

    0

    0

    0.0239

    As1

    6g

    0.2417(8)

    0

    1/4

    0.0173

    As2

    4d

    1/3

    2/3

    0

    0.0285

    Space group: P63/mcm—hexagonal (No.193); a=8.9845(1) Å, c=5.8897(1) Å; V=411.73(1) Å3; χ2=2.9, Rp=2.5%, Rwp=4.9%.

  • Table 2   Selected distances between adjacent atoms and angles

    Selected atom

    Distance (Å)and angle (°)

    Selected atom

    Distance (Å)and angle (°)

    La–As1(×2)

    3.1864(1)

    La–La

    3.6795(7)

    La–As2(×4)

    3.1799(1)

    As2–As2a

    5.1873(0)

    La–As1(×2)

    2.9738(5)

    Cr–As1

    2.6243(1)

    Cr–Cr (×2)a

    2.9448(1)

    As1–Cr–As1

    88.408(5)

    Cr–Crb

    8.9845(1)

    91.592(6)

    The intrachain distance; b) the interchain distance.

  • Table 3   Selected interactions, their distances after structure relaxation and their corresponding ICOHPs per bond in La3CrAs5

    Interaction

    Distance (Å)

    ICOHP per bond (eV)

    Cr–Cr

    2.986

    −0.82

    Cr–As1

    2.616

    −1.42

    La–As1

    2.998

    −1.74

    La–As2

    3.215

    −1.53

    As2–As2

    2.986

    −1.58

    La–La

    3.804

    −0.96

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