Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagram
We present a combined experimental and theoretical study on the quasi-one-dimensional organic conductor (TMTTF)_{2}PF_{6}, and elucidate the variation of its physical properties under pressure. We fully resolve the crystal structure by single crystal x-ray diffraction measurements using a diamond an...
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| Language: | English |
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American Physical Society
2024-12-01
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| Series: | Physical Review Research |
| Online Access: | http://doi.org/10.1103/PhysRevResearch.6.043308 |
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| author | Miho Itoi Kazuyoshi Yoshimi Hanming Ma Takahiro Misawa Takao Tsumuraya Dilip Bhoi Tokutaro Komatsu Hatsumi Mori Yoshiya Uwatoko Hitoshi Seo |
| author_facet | Miho Itoi Kazuyoshi Yoshimi Hanming Ma Takahiro Misawa Takao Tsumuraya Dilip Bhoi Tokutaro Komatsu Hatsumi Mori Yoshiya Uwatoko Hitoshi Seo |
| author_sort | Miho Itoi |
| collection | DOAJ |
| description | We present a combined experimental and theoretical study on the quasi-one-dimensional organic conductor (TMTTF)_{2}PF_{6}, and elucidate the variation of its physical properties under pressure. We fully resolve the crystal structure by single crystal x-ray diffraction measurements using a diamond anvil cell up to 8 GPa, and based on the structural data, we perform first-principles density-functional theory calculations and derive the ab initio extended Hubbard-type Hamiltonians. Furthermore, we compare the behavior of the resistivity measured up to 3 GPa using a BeCu clamp-type cell and the ground state properties of the obtained model numerically calculated by the many-variable variational Monte Carlo method. Our main findings are as follows: (i) The crystal was rapidly compressed up to about 3 GPa where the volume drops to 80% and gradually varies down to 70% at 8 GPa. The transfer integrals increase following such behavior whereas the screened Coulomb interactions decrease, resulting in a drastic reduction of correlation effect. (ii) The degree of dimerization in the intrachain transfer integrals, as the result of the decrease in structural dimerization together with the change in the intermolecular configuration, almost disappears above 4 GPa; the interchain transfer integrals also show characteristic variations under pressure. (iii) The results of identifying the characteristic temperatures in the resistivity and the charge and spin orderings in the calculations show an overall agreement: The charge ordering sensitively becomes unstable above 1 GPa, while the spin ordering survives up to higher pressures. These results shed light on the similarities and differences between applying external pressure and substituting the chemical species (chemical pressure). |
| format | Article |
| id | doaj-art-99e58ca97ee9400bb6cebd6ed5b9c807 |
| institution | OA Journals |
| issn | 2643-1564 |
| language | English |
| publishDate | 2024-12-01 |
| publisher | American Physical Society |
| record_format | Article |
| series | Physical Review Research |
| spelling | doaj-art-99e58ca97ee9400bb6cebd6ed5b9c8072025-08-20T01:59:49ZengAmerican Physical SocietyPhysical Review Research2643-15642024-12-016404330810.1103/PhysRevResearch.6.043308Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagramMiho ItoiKazuyoshi YoshimiHanming MaTakahiro MisawaTakao TsumurayaDilip BhoiTokutaro KomatsuHatsumi MoriYoshiya UwatokoHitoshi SeoWe present a combined experimental and theoretical study on the quasi-one-dimensional organic conductor (TMTTF)_{2}PF_{6}, and elucidate the variation of its physical properties under pressure. We fully resolve the crystal structure by single crystal x-ray diffraction measurements using a diamond anvil cell up to 8 GPa, and based on the structural data, we perform first-principles density-functional theory calculations and derive the ab initio extended Hubbard-type Hamiltonians. Furthermore, we compare the behavior of the resistivity measured up to 3 GPa using a BeCu clamp-type cell and the ground state properties of the obtained model numerically calculated by the many-variable variational Monte Carlo method. Our main findings are as follows: (i) The crystal was rapidly compressed up to about 3 GPa where the volume drops to 80% and gradually varies down to 70% at 8 GPa. The transfer integrals increase following such behavior whereas the screened Coulomb interactions decrease, resulting in a drastic reduction of correlation effect. (ii) The degree of dimerization in the intrachain transfer integrals, as the result of the decrease in structural dimerization together with the change in the intermolecular configuration, almost disappears above 4 GPa; the interchain transfer integrals also show characteristic variations under pressure. (iii) The results of identifying the characteristic temperatures in the resistivity and the charge and spin orderings in the calculations show an overall agreement: The charge ordering sensitively becomes unstable above 1 GPa, while the spin ordering survives up to higher pressures. These results shed light on the similarities and differences between applying external pressure and substituting the chemical species (chemical pressure).http://doi.org/10.1103/PhysRevResearch.6.043308 |
| spellingShingle | Miho Itoi Kazuyoshi Yoshimi Hanming Ma Takahiro Misawa Takao Tsumuraya Dilip Bhoi Tokutaro Komatsu Hatsumi Mori Yoshiya Uwatoko Hitoshi Seo Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagram Physical Review Research |
| title | Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagram |
| title_full | Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagram |
| title_fullStr | Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagram |
| title_full_unstemmed | Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagram |
| title_short | Combined x-ray diffraction, electrical resistivity, and ab initio study of (TMTTF)_{2}PF_{6} under pressure: Implications for the unified phase diagram |
| title_sort | combined x ray diffraction electrical resistivity and ab initio study of tmttf 2 pf 6 under pressure implications for the unified phase diagram |
| url | http://doi.org/10.1103/PhysRevResearch.6.043308 |
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