Gapless spinons and a field-induced soliton gap in the hyper-honeycomb Cu oxalate framework compound [(C$_{2}$H$_{5}$)$_{3}$NH]$_{2}$Cu$_{2}$(C$_{2}$O$_{4}$)$_{3}$
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| Main Authors: | , , , , , , , , , , , , , , , , |
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| Format: | Preprint |
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2023
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| author | Dissanayake, C. Jacko, A. C. Kumarasinghe, K. Munir, R. Siddiquee, H. Newsome, W. J. Uribe-Romo, F. J. Choi, E. S. Yadav, S. Hu, X. -Z. Takano, Y. Pakhira, S. Johnston, D. C. Ding, Q. -P. Furukawa, Y. Powell, B. J. Nakajima, Y. |
| author_facet | Dissanayake, C. Jacko, A. C. Kumarasinghe, K. Munir, R. Siddiquee, H. Newsome, W. J. Uribe-Romo, F. J. Choi, E. S. Yadav, S. Hu, X. -Z. Takano, Y. Pakhira, S. Johnston, D. C. Ding, Q. -P. Furukawa, Y. Powell, B. J. Nakajima, Y. |
| contents | We report a detailed study of the specific heat and magnetic susceptibility of single crystals of a spin liquid candidate: the hyper-honeycomb Cu oxalate framework compound [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$. The specific heat shows no anomaly associated with a magnetic transition at low temperatures down to $T\sim$ 180 mK in zero magnetic field. We observe a large linear-in-$T$ contribution to the specific heat $γT$, $γ= 98(1)$ mK/mol K$^{2}$, at low temperatures, indicative of the presence of fermionic excitations despite the Mott insulating state. The low-$T$ specific heat is strongly suppressed by applied magnetic fields $H$, which induce an energy gap, $Δ(H)$, in the spin-excitation spectrum. We use the four-component relativistic density-functional theory (DFT) to calculate the magnetic interactions, including the Dzyaloshinskii-Moriya antisymmetric exchange, which causes an effective staggered field acting on one copper sublattice. The magnitude and field dependence of the field-induced gap, $Δ(H) \propto H^{2/3}$, are accurately predicted by the soliton mass calculated from the sine-Gordon model of weakly coupled antiferromagnetic Heisenberg chains with all parameters determined by our DFT calculations. Thus our experiment and calculations are entirely consistent with a model of [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ in which anisotropic magnetic exchange interactions due to Jahn-Teller distortion cause one copper sublattice to dimerize, leaving a second sublattice of weakly coupled antiferromagnetic chains. We also show that this model quantitatively accounts for the measured temperature-dependent magnetic susceptibility. Thus [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ is a canonical example of a one-dimensional spin-1/2 Heisenberg antiferromagnet and not a resonating-valence-bond quantum spin liquid, as previously proposed. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2306_13598 |
| institution | arXiv |
| publishDate | 2023 |
| record_format | arxiv |
| spellingShingle | Gapless spinons and a field-induced soliton gap in the hyper-honeycomb Cu oxalate framework compound [(C$_{2}$H$_{5}$)$_{3}$NH]$_{2}$Cu$_{2}$(C$_{2}$O$_{4}$)$_{3}$ Dissanayake, C. Jacko, A. C. Kumarasinghe, K. Munir, R. Siddiquee, H. Newsome, W. J. Uribe-Romo, F. J. Choi, E. S. Yadav, S. Hu, X. -Z. Takano, Y. Pakhira, S. Johnston, D. C. Ding, Q. -P. Furukawa, Y. Powell, B. J. Nakajima, Y. Strongly Correlated Electrons We report a detailed study of the specific heat and magnetic susceptibility of single crystals of a spin liquid candidate: the hyper-honeycomb Cu oxalate framework compound [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$. The specific heat shows no anomaly associated with a magnetic transition at low temperatures down to $T\sim$ 180 mK in zero magnetic field. We observe a large linear-in-$T$ contribution to the specific heat $γT$, $γ= 98(1)$ mK/mol K$^{2}$, at low temperatures, indicative of the presence of fermionic excitations despite the Mott insulating state. The low-$T$ specific heat is strongly suppressed by applied magnetic fields $H$, which induce an energy gap, $Δ(H)$, in the spin-excitation spectrum. We use the four-component relativistic density-functional theory (DFT) to calculate the magnetic interactions, including the Dzyaloshinskii-Moriya antisymmetric exchange, which causes an effective staggered field acting on one copper sublattice. The magnitude and field dependence of the field-induced gap, $Δ(H) \propto H^{2/3}$, are accurately predicted by the soliton mass calculated from the sine-Gordon model of weakly coupled antiferromagnetic Heisenberg chains with all parameters determined by our DFT calculations. Thus our experiment and calculations are entirely consistent with a model of [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ in which anisotropic magnetic exchange interactions due to Jahn-Teller distortion cause one copper sublattice to dimerize, leaving a second sublattice of weakly coupled antiferromagnetic chains. We also show that this model quantitatively accounts for the measured temperature-dependent magnetic susceptibility. Thus [(C$_2$H$_5$)$_3$NH]$_2$Cu$_2$(C$_2$O$_4$)$_3$ is a canonical example of a one-dimensional spin-1/2 Heisenberg antiferromagnet and not a resonating-valence-bond quantum spin liquid, as previously proposed. |
| title | Gapless spinons and a field-induced soliton gap in the hyper-honeycomb Cu oxalate framework compound [(C$_{2}$H$_{5}$)$_{3}$NH]$_{2}$Cu$_{2}$(C$_{2}$O$_{4}$)$_{3}$ |
| topic | Strongly Correlated Electrons |
| url | https://arxiv.org/abs/2306.13598 |