The Zn1−xPbxCr2Se4—Single Crystals Obtained by Chemical Vapour Transport—Structure and Magnetic, Electrical, and Thermal Properties
Abstract
:1. Introduction
2. Materials and Methods
2.1. Computation of Thermodynamic Parameters for the Chemical Transport Reactions
- 2ZnSe + 4CrCl3(g) = 2ZnCl2(g) + 4CrCl2(g) + Se2(g)
- 2ZnSe + 4CrCl3(g) = Zn2Cl4(g) + 4CrCl2(g) + Se2(g)
- 2PbSe + 2CrCl3(g) = 2PbCl(g) + 2CrCl2(g) + Se2(g)
- 2PbSe + 4CrCl3(g) = 2PbCl2(g) + 4CrCl2(g) + Se2(g)
- 2ZnSe + 2CrCl4(g) = 2ZnCl2(g) + 2CrCl2(g) + Se2(g)
- 2ZnSe + 2CrCl4(g) = Zn2Cl4(g) + 2CrCl2(g) + Se2(g)
- 2PbSe + CrCl4(g) = 2PbCl(g) + CrCl2(g) + Se2(g)
- 2PbSe + 2CrCl4(g) = 2PbCl2(g) + 2CrCl2(g) + Se2(g)
- 2ZnSe + 2Cl2(g) = 2ZnCl2(g) + Se2(g)
- 2ZnSe + 2Cl2(g) = Zn2Cl4(g) + Se2(g)
- 2PbSe + Cl2(g) = 2PbCl(g) + Se2(g)
- 2PbSe + 2Cl2(g) = 2PbCl2(g) + Se2(g)
2.2. Synthesis of ZnSe and PbSe
2.3. Crystal Structure and Chemical Composition
2.4. Magnetic and Electrical Measurements
3. Results and Discussion
3.1. Growth of Single Crystals and Chemical Composition
3.2. Structural Study
3.3. Electrical and Magnetic Properties
3.4. Specific Heat Studies
3.5. Thermal Analysis
4. Conclusions
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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No | Amounts of Substrates (mmol) | Td (K) | Tc (K) | ΔT (K) | % Weight | Chemical Formula | ||||
---|---|---|---|---|---|---|---|---|---|---|
nZnSe | nPbSe | Zn | Pb | Cr | Se | |||||
(1) | 14.4 | 1.6 | 1223 | 1163 | 60 | 12.31 ± 0.09 | 3.23 ± 0.06 | 20.66 ± 0.01 | 63.71 ± 0.04 | Zn0.94Pb0.06Cr2Se4 |
(2) | 14.4 | 1.6 | 1133 | 1083 | 50 | 12.25 ± 0.08 | 2.95 ± 0.07 | 20.45 ± 0.02 | 64.54 ± 0.05 | Zn0.92Pb0.07Cr2Se4 |
(3) | 12.8 | 3.2 | 1203 | 1153 | 50 | 12.05 ± 0.06 | 3.43 ± 0.06 | 20.49 ± 0.05 | 64.10 ± 0.03 | Zn0.92Pb0.09Cr2Se4 |
(4) | 12.8 | 3.2 | 1203 | 1143 | 60 | 11.63 ± 0.02 | 4.51 ± 0.04 | 20.30 ± 0.06 | 63.56 ± 0.03 | Zn0.89Pb0.11Cr2Se4 |
(5) | 11.2 | 4.8 | 1203 | 1153 | 50 | 11.42 ± 0.03 | 4.98 ± 0.05 | 20.15 ± 0.03 | 63.42 ± 0.03 | Zn0.88Pb0.12Cr2Se4 |
Chemical Formula | Lattice Parameter (Å) | Volume (Å3) | Density Calc. (Mg/m3) | Absorption Coeff. (mm−1) | Goodness of Fit on F2 | R Parameters | |
---|---|---|---|---|---|---|---|
R1 | wR2 | ||||||
Zn0.94Pb0.06Cr2Se4 | 10.4910(3) | 1154.65(2) | 5.682 | 32.837 | 1.150 | 0.0223 | 0.0662 |
Zn0.92Pb0.07Cr2Se4 | 10.4933(2) | 1155.41(3) | 5.689 | 32.883 | 1.205 | 0.0333 | 0.1114 |
Zn0.92Pb0.09Cr2Se4 | 10.4946(4) | 1155.84(1) | 5.709 | 32.856 | 1.175 | 0.0261 | 0.0839 |
Zn0.89Pb0.11Cr2Se4 | 10.4954(2) | 1156.10(2) | 5.757 | 33.841 | 1.196 | 0.0333 | 0.1114 |
Zn0.88Pb0.12Cr2Se4 | 10.4959(1) | 1156.27(3) | 5.772 | 33.852 | 1.191 | 0.0311 | 0.1012 |
Spinel | Anion Parameter u | Site Occupation | Uiso (Å × 103) | |||
---|---|---|---|---|---|---|
(A) | (B) | Zn/Pb | Cr | Se | ||
(Zn0.94Pb0.06)[Cr2]Se4 | 0.2595(1) | 0.94(1):0.06(1) | 1.0 | 13(1) | 7(1) | 7(1) |
(Zn0.92Pb0.07)[Cr2]Se4 | 0.2595(1) | 0.92(2):0.07(1) | 1.0 | 14(1) | 6(1) | 6(1) |
(Zn0.92Pb0.09)[Cr2]Se4 | 0.2595(1) | 0.92(1):0.09(1) | 1.0 | 13(1) | 7(1) | 6(1) |
(Zn0.89Pb0.11)[Cr2]Se4 | 0.2595(1) | 0.89(2):0.11(2) | 1.0 | 14(1) | 5(1) | 5(1) |
(Zn0.88Pb0.12)[Cr2]Se4 | 0.2595(1) | 0.87(1):0.13(2) | 1.0 | 14(1) | 5(1) | 6(1) |
Spinel | Bond Distances | Bond Angles | ||
---|---|---|---|---|
Zn/Pb–Se | Cr–Se | Se–Zn/Pb–Se | Se–Cr–Se | |
(Zn0.94Pb0.06)[Cr2]Se4 | 2.4451(5) | 2.5282(3) | 109.5(0) × 6 | 180.0(0) × 3 94.61(13) × 6 85.39(13) × 6 |
(Zn0.92Pb0.07)[Cr2]Se4 | 2.4442(7) | 2.5269(4) | 109.5(0) × 6 | 180.0(0) × 3 94.61(2) × 6 85.39(2) × 6 |
(Zn0.92Pb0.09)[Cr2]Se4 | 2.4453(5) | 2.5274(3) | 109.5(0) × 6 | 180.0(0) × 3 94.62(14) × 6 85.38(14) × 6 |
(Zn0.89Pb0.11)[Cr2]Se4 | 2.4453(8) | 2.5279(4) | 109.5(0) × 6 | 180.0(0) × 3 94.62(2) × 6 82.38(2) × 6 |
(Zn0.88Pb0.12)[Cr2]Se4 | 2.4453(7) | 2.5280(4) | 109.5(0) × 6 | 180.0(0) × 3 94.61(2) × 6 85.39(2) × 6 |
Spinel | C | TN | θ | µeff | Ms(2K) | J1 | J2 | Hc1 | Hc2 | Ea |
---|---|---|---|---|---|---|---|---|---|---|
(emu·K/mol) | (K) | (K) | (µB/f.u.) | (µB/f.u.) | (K) | (K) | (kOe) | (kOe) | (eV) | |
ZnCr2Se4 | 4.082 | 21 | 90 | 5.714 | 6.0 | −1.65 | 1.28 | 10.0 | 65.0 | 0.135 |
Zn0.94Pb0.06Cr2Se4 | 5.477 | 22 | 74 | 6.618 | 5.325 | −2.07 | 1.17 | 12.0 | 55.0 | 0.138 |
Zn0.92Pb0.07Cr2Se4 | 5.568 | 22 | 77 | 6.673 | 5.964 | −1.95 | 1.23 | 12.0 | 56.0 | 0.161 |
Zn0.92Pb0.09Cr2Se4 | 4.727 | 22 | 81 | 6.149 | 5.960 | −2.02 | 1.19 | 12.0 | 61.0 | 0.146 |
Zn0.89Pb0.11Cr2Se4 | 5.768 | 22 | 83 | 6.792 | 5.486 | −1.92 | 1.24 | 12.0 | 55.0 | 0.177 |
Zn0.88Pb0.12Cr2Se4 | 5.898 | 22 | 84 | 6.868 | 5.251 | −1.90 | 1.25 | 12.0 | 57.0 | 0.315 |
Spinel | Hdc | C | TN | θ | Tm | µeff | J1 | J2 |
---|---|---|---|---|---|---|---|---|
(kOe) | (emu·K/mol) | (K) | (K) | (K) | (µB/f.u.) | (K) | (K) | |
Zn0.94Pb0.06Cr2Se4 | 0 | 5.477 | 22 | 74 | - | 6.618 | −2.07 | 1.17 |
10 | 4.211 | 22 | 76 | - | 5.803 | −1.73 | 1.13 | |
20 | 4.086 | 18 | 79 | - | 5.716 | −1.38 | 1.11 | |
30 | 3.986 | 16 | 82 | - | 5.646 | −1.03 | 1.08 | |
40 | 3.948 | 12 | 95 | 31.5 | 5.619 | 0.22 | 1.09 | |
50 | 3.863 | 6 | 108 | 46 | 5.558 | 0.90 | 1.05 | |
Zn0.92Pb0.07Cr2Se4 | 0 | 5.568 | 22 | 77 | - | 6.673 | −1.95 | 1.23 |
10 | 4.182 | 20 | 78 | - | 5.783 | −1.6 | 1.18 | |
20 | 4.102 | 19 | 81 | - | 5.728 | −1.45 | 1.18 | |
30 | 4.003 | 16 | 84 | - | 5.658 | −0.9 | 1.11 | |
40 | 3.988 | 12 | 96 | 33 | 5.648 | −0.18 | 1.11 | |
50 | 3.976 | 7 | 99 | 44 | 5.639 | 0.60 | 1.00 | |
Zn0.92Pb0.09Cr2Se4 | 0 | 4.727 | 22 | 81 | - | 6.149 | −2.02 | 1.19 |
10 | 3.922 | 21 | 82 | - | 5.601 | −1.85 | 1.18 | |
20 | 3.711 | 20 | 84 | - | 5.448 | −1.65 | 1.17 | |
30 | 3.681 | 16 | 85 | - | 5.426 | −1.00 | 1.10 | |
40 | 3.602 | 12 | 97 | 33.5 | 5.367 | −0.20 | 1.10 | |
50 | 3.639 | 6 | 108 | 46 | 5.369 | 0.90 | 1.05 | |
Zn0.89Pb0.11Cr2Se4 | 0 | 5.768 | 22 | 83 | - | 6.792 | −1.92 | 1.24 |
10 | 4.293 | 20 | 84 | - | 5.859 | −1.60 | 1.20 | |
20 | 4.182 | 19 | 85 | - | 5.783 | −1.4 | 1.18 | |
30 | 4.101 | 16 | 86 | - | 5.727 | −0.97 | 1.12 | |
40 | 4.056 | 12 | 91 | 34 | 5.695 | −0.28 | 1.06 | |
50 | 4.002 | 6 | 97 | 48 | 5.657 | 0.72 | 0.96 | |
Zn0.88Pb0.12Cr2Se4 | 0 | 5.898 | 22 | 84 | - | 6.868 | −1.90 | 1.25 |
10 | 3.794 | 20 | 86 | - | 5.508 | −1.57 | 1.22 | |
20 | 3.781 | 19 | 88 | - | 5.499 | −1.38 | 1.21 | |
30 | 3.762 | 16 | 90 | - | 5.485 | −0.90 | 1.15 | |
40 | 3.703 | 12 | 94 | 36 | 5.442 | −0.23 | 1.08 | |
50 | 3.689 | 6 | 98 | 48 | 5.432 | 0.73 | 0.97 |
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Jendrzejewska, I.; Groń, T.; Kusz, J.; Stokłosa, Z.; Pietrasik, E.; Goryczka, T.; Sawicki, B.; Goraus, J.; Jampilek, J.; Duda, H.; et al. The Zn1−xPbxCr2Se4—Single Crystals Obtained by Chemical Vapour Transport—Structure and Magnetic, Electrical, and Thermal Properties. Materials 2022, 15, 5289. https://doi.org/10.3390/ma15155289
Jendrzejewska I, Groń T, Kusz J, Stokłosa Z, Pietrasik E, Goryczka T, Sawicki B, Goraus J, Jampilek J, Duda H, et al. The Zn1−xPbxCr2Se4—Single Crystals Obtained by Chemical Vapour Transport—Structure and Magnetic, Electrical, and Thermal Properties. Materials. 2022; 15(15):5289. https://doi.org/10.3390/ma15155289
Chicago/Turabian StyleJendrzejewska, Izabela, Tadeusz Groń, Joachim Kusz, Zbigniew Stokłosa, Ewa Pietrasik, Tomasz Goryczka, Bogdan Sawicki, Jerzy Goraus, Josef Jampilek, Henryk Duda, and et al. 2022. "The Zn1−xPbxCr2Se4—Single Crystals Obtained by Chemical Vapour Transport—Structure and Magnetic, Electrical, and Thermal Properties" Materials 15, no. 15: 5289. https://doi.org/10.3390/ma15155289