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| Main Authors: | , , , , , |
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| Format: | Preprint |
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2024
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| Subjects: | |
| Online Access: | https://arxiv.org/abs/2412.16103 |
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| _version_ | 1866915074016280576 |
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| author | Deltsidis, Alexandros Kaitatzi, Myrsini Simonelli, Laura Stock, Chris Voneshen, David Lappas, Alexandros |
| author_facet | Deltsidis, Alexandros Kaitatzi, Myrsini Simonelli, Laura Stock, Chris Voneshen, David Lappas, Alexandros |
| contents | Intercalation of two-dimensional (2D) iron chalcogenides with molecular species requires disentangling electronic and structural contributions to understand the puzzling limit to superconducting transition temperature ($T_c$) at the frontier of long interlayer separations. Here, synchrotron X-ray absorption spectroscopy (XAS) at the Se K-edge sheds light on the impact of carrier-doping on the local structure of the high-$T_c$ (~39 K) $Li_{1.0}(C_5H_5N)_yFe_{2-z}Se_2$ phase. This material is derived by annealing the structurally related as-made derivative ($T_c$~ 44 K), with layers being primed apart by [alkali-molecule] guests. Metrics, such as, a reduced filling of Se $4p$ orbitals and shorter Fe-Se bonds in the annealed phase, corroborate to a lower electron doping level with respect to the as-made one. Analysis of the metal-ligand thermal motion, based on the correlated Debye model, further relates the higher $T_c$ intercalates with the softening of the local Fe-Se bond. Beyond electronic effects, intercalation brings forth host-guest interactions that mediate the dynamics of the bulk crystal structure. For this, neutron time-of-flight spectroscopy on the annealed derivative, corroborates to the Se-Fe-Se layer being sensitive to chemical pressure effects imposed by the confined organic guests. This reflects in the phonon density of states, where harder low-energy transverse acoustic matrix phonons and molecular vibrations are witnessed, with respect to the pristine inorganic ($β$-FeSe) and organic ($C_5D_5N$) counterparts. On cooling through $T_c$, these excitations arrive without a collective magnetic-resonance mode - essential in unconventional, spin-mediated mechanisms - enquiring about deviations from optimal doping. The work highlights that when the Fe-square planes are tuned far apart, carrier-doping leveraged by intercalation plays a key role in the $T_c$ parametrization. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2412_16103 |
| institution | arXiv |
| publishDate | 2024 |
| record_format | arxiv |
| spellingShingle | Local structure and phonon states mediated by intercalation-driven doping in superconducting $Li_{1.0}(C_5H_5N)_yFe_{2-z}Se_2$ Deltsidis, Alexandros Kaitatzi, Myrsini Simonelli, Laura Stock, Chris Voneshen, David Lappas, Alexandros Superconductivity Materials Science Strongly Correlated Electrons Intercalation of two-dimensional (2D) iron chalcogenides with molecular species requires disentangling electronic and structural contributions to understand the puzzling limit to superconducting transition temperature ($T_c$) at the frontier of long interlayer separations. Here, synchrotron X-ray absorption spectroscopy (XAS) at the Se K-edge sheds light on the impact of carrier-doping on the local structure of the high-$T_c$ (~39 K) $Li_{1.0}(C_5H_5N)_yFe_{2-z}Se_2$ phase. This material is derived by annealing the structurally related as-made derivative ($T_c$~ 44 K), with layers being primed apart by [alkali-molecule] guests. Metrics, such as, a reduced filling of Se $4p$ orbitals and shorter Fe-Se bonds in the annealed phase, corroborate to a lower electron doping level with respect to the as-made one. Analysis of the metal-ligand thermal motion, based on the correlated Debye model, further relates the higher $T_c$ intercalates with the softening of the local Fe-Se bond. Beyond electronic effects, intercalation brings forth host-guest interactions that mediate the dynamics of the bulk crystal structure. For this, neutron time-of-flight spectroscopy on the annealed derivative, corroborates to the Se-Fe-Se layer being sensitive to chemical pressure effects imposed by the confined organic guests. This reflects in the phonon density of states, where harder low-energy transverse acoustic matrix phonons and molecular vibrations are witnessed, with respect to the pristine inorganic ($β$-FeSe) and organic ($C_5D_5N$) counterparts. On cooling through $T_c$, these excitations arrive without a collective magnetic-resonance mode - essential in unconventional, spin-mediated mechanisms - enquiring about deviations from optimal doping. The work highlights that when the Fe-square planes are tuned far apart, carrier-doping leveraged by intercalation plays a key role in the $T_c$ parametrization. |
| title | Local structure and phonon states mediated by intercalation-driven doping in superconducting $Li_{1.0}(C_5H_5N)_yFe_{2-z}Se_2$ |
| topic | Superconductivity Materials Science Strongly Correlated Electrons |
| url | https://arxiv.org/abs/2412.16103 |