Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I)
In this study, we theoretically investigate the structural, electronic and magnetic properties of the Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) compounds. Previous studies reported potential spin-driven ferroelectricity in Cu<sub>2</sub>OCl<sub>2</sub&...
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MDPI AG
2022-05-01
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| Online Access: | https://www.mdpi.com/2079-3197/10/5/73 |
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| author | William Lafargue-Dit-Hauret Xavier Rocquefelte |
| author_facet | William Lafargue-Dit-Hauret Xavier Rocquefelte |
| author_sort | William Lafargue-Dit-Hauret |
| collection | DOAJ |
| description | In this study, we theoretically investigate the structural, electronic and magnetic properties of the Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) compounds. Previous studies reported potential spin-driven ferroelectricity in Cu<sub>2</sub>OCl<sub>2</sub>, originating from a non-collinear magnetic phase existing below <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula>∼70 K. However, the nature of this low-temperature magnetic phase is still under debate. Here, we focus on the calculation of <i>J</i> exchange couplings and enhance knowledge in the field by (i) characterizing the low-temperature magnetic order for Cu<sub>2</sub>OCl<sub>2</sub> and (ii) evaluating the impact of the chemical pressure on the magnetic interactions, which leads us to consider the two new phases Cu<sub>2</sub>OBr<sub>2</sub> and Cu<sub>2</sub>OI<sub>2</sub>. Our <i>ab initio</i> simulations notably demonstrate the coexistence of strong antiferromagnetic and ferromagnetic interactions, leading to spin frustration. The <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> Néel temperatures were estimated on the basis of a quasi-1D AFM model using the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mrow><mi mathvariant="italic">ab</mi><mi mathvariant="italic">initio</mi></mrow></mrow></semantics></math></inline-formula><i>J</i> couplings. It nicely reproduces the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> value for Cu<sub>2</sub>OCl<sub>2</sub> and allows us to predict an increase of <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> under chemical pressure, with <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> = 120 K for the dynamically stable phase Cu<sub>2</sub>OBr<sub>2</sub>. This investigation suggests that chemical pressure is an effective key factor to open the door of room-temperature multiferroicity. |
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| spelling | doaj.art-a31d6eaef63f477daca02c84dbb757562023-11-23T10:33:20ZengMDPI AGComputation2079-31972022-05-011057310.3390/computation10050073Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I)William Lafargue-Dit-Hauret0Xavier Rocquefelte1Univ Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226, F-35000 Rennes, FranceUniv Rennes, CNRS, ISCR (Institut des Sciences Chimiques de Rennes) UMR 6226, F-35000 Rennes, FranceIn this study, we theoretically investigate the structural, electronic and magnetic properties of the Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) compounds. Previous studies reported potential spin-driven ferroelectricity in Cu<sub>2</sub>OCl<sub>2</sub>, originating from a non-collinear magnetic phase existing below <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula>∼70 K. However, the nature of this low-temperature magnetic phase is still under debate. Here, we focus on the calculation of <i>J</i> exchange couplings and enhance knowledge in the field by (i) characterizing the low-temperature magnetic order for Cu<sub>2</sub>OCl<sub>2</sub> and (ii) evaluating the impact of the chemical pressure on the magnetic interactions, which leads us to consider the two new phases Cu<sub>2</sub>OBr<sub>2</sub> and Cu<sub>2</sub>OI<sub>2</sub>. Our <i>ab initio</i> simulations notably demonstrate the coexistence of strong antiferromagnetic and ferromagnetic interactions, leading to spin frustration. The <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> Néel temperatures were estimated on the basis of a quasi-1D AFM model using the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><mrow><mrow><mi mathvariant="italic">ab</mi><mi mathvariant="italic">initio</mi></mrow></mrow></semantics></math></inline-formula><i>J</i> couplings. It nicely reproduces the <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> value for Cu<sub>2</sub>OCl<sub>2</sub> and allows us to predict an increase of <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> under chemical pressure, with <inline-formula><math xmlns="http://www.w3.org/1998/Math/MathML" display="inline"><semantics><msub><mi>T</mi><mi>N</mi></msub></semantics></math></inline-formula> = 120 K for the dynamically stable phase Cu<sub>2</sub>OBr<sub>2</sub>. This investigation suggests that chemical pressure is an effective key factor to open the door of room-temperature multiferroicity.https://www.mdpi.com/2079-3197/10/5/73Cu<sub>2</sub>OCl<sub>2</sub>Cu<sub>2</sub>OBr<sub>2</sub>Cu<sub>2</sub>OI<sub>2</sub>oxyhalidesdensity functional theorymagnetic couplings |
| spellingShingle | William Lafargue-Dit-Hauret Xavier Rocquefelte Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) Computation Cu<sub>2</sub>OCl<sub>2</sub> Cu<sub>2</sub>OBr<sub>2</sub> Cu<sub>2</sub>OI<sub>2</sub> oxyhalides density functional theory magnetic couplings |
| title | Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) |
| title_full | Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) |
| title_fullStr | Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) |
| title_full_unstemmed | Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) |
| title_short | Influence of the Chemical Pressure on the Magnetic Properties of the Mixed Anion Cuprates Cu<sub>2</sub>OX<sub>2</sub> (X = Cl, Br, I) |
| title_sort | influence of the chemical pressure on the magnetic properties of the mixed anion cuprates cu sub 2 sub ox sub 2 sub x cl br i |
| topic | Cu<sub>2</sub>OCl<sub>2</sub> Cu<sub>2</sub>OBr<sub>2</sub> Cu<sub>2</sub>OI<sub>2</sub> oxyhalides density functional theory magnetic couplings |
| url | https://www.mdpi.com/2079-3197/10/5/73 |
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