Electronic state of a new organic conductor (TTM-TTP)I3 with a one-dimensional half-filled band

Onuki, Masamichi; Hiraki, K.; Takahashi, Toshihiro; Jinno, D.; Kawamoto, Tadashi; Mori, Takehiko; Tanaka, Kazuyoshi; Misaki, Y.

doi:10.1016/s0022-3697(00)00176-1

Cited by 17 publications

(13 citation statements)

References 4 publications

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“…On the basis of this finding, we infer that the non-magnetic insulating behavior observed at low temperatures in (TTM-TTP)I 3 (Refs. [31][32][33][34] can be attributed to the spin-singlet formation on the t with twofold periodicity along the stacking direction. Incidentally, we observe that the IAF state is almost degenerate with the ICO state, with the energy differences per molecule E IAF − E ICO ≈ 0.15 eV, E SDW − E ICO ≈ 0.30 eV, and E CDW − E ICO ≈ 1.19 eV.…”

Section: Full Fragment Decompositionmentioning

confidence: 99%

“…[31][32][33][34] A charge ordering reflected by the alternation of valence of TTM-TTP molecule along the stacking direction has been proposed initially. 33,34 The experimental analysis based on Raman-scattering [35][36][37] and x-ray 38 measurements suggested a new type of charge-ordered state, "intra-molecular charge ordering (ICO)," which cannot be described by the conventional single-orbital approximation. By performing wavefunction-based ab initio calculations for the isolated ionic TTM-TTP molecule, 29 we previously revealed that this system has a multiconfigurational character.…”

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confidence: 99%

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Ab initio derivation of multi-orbital extended Hubbard model for molecular crystals

Tsuchiizu

Omori

Suzumura

et al. 2012

The Journal of Chemical Physics

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From configuration interaction (CI) ab initio calculations, we derive an effective two-orbital extended Hubbard model based on the gerade (g) and ungerade (u) molecular orbitals (MOs) of the chargetransfer molecular conductor (TTM-TTP)I-3 and the single-component molecular conductor Au(tmdt)(2)]. First, by focusing on the isolated molecule, we determine the parameters for the model Hamiltonian so as to reproduce the CI Hamiltonian matrix. Next, we extend the analysis to two neighboring molecule pairs in the crystal and we perform similar calculations to evaluate the intermolecular interactions. From the resulting tight-binding parameters, we analyze the band structure to confirm that two bands overlap and mix in together, supporting the multi-band feature. Furthermore, using a fragment decomposition, we derive the effective model based on the fragment MOs and show that the staking TTM-TTP molecules can be described by the zig-zag two-leg ladder with the inter-molecular transfer integral being larger than the intra-fragment transfer integral within the molecule. The inter-site interactions between the fragments follow a Coulomb law, supporting the fragment decomposition strategy. . First, by focusing on the isolated molecule, we determine the parameters for the model Hamiltonian so as to reproduce the CI Hamiltonian matrix. Next, we extend the analysis to two neighboring molecule pairs in the crystal and we perform similar calculations to evaluate the intermolecular interactions. From the resulting tight-binding parameters, we analyze the band structure to confirm that two bands overlap and mix in together, supporting the multi-band feature. Furthermore, using a fragment decomposition, we derive the effective model based on the fragment MOs and show that the staking TTM-TTP molecules can be described by the zig-zag two-leg ladder with the inter-molecular transfer integral being larger than the intra-fragment transfer integral within the molecule. The inter-site interactions between the fragments follow a Coulomb law, supporting the fragment decomposition strategy.

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Section: Full Fragment Decompositionmentioning

confidence: 99%

mentioning

confidence: 99%

Ab initio derivation of multi-orbital extended Hubbard model for molecular crystals

Tsuchiizu

Omori

Suzumura

et al. 2012

The Journal of Chemical Physics

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“…A tight-binding band calculation suggests that (TTM-TTP)I 3 has a large bandwidth of W = 1 eV. The nature of the insulating state of (TTM-TTP)I 3 has been investigated, but has not get been elucidated [76][77][78][79][80][81]. On the other hand, (TTM-TTP)(I 3 ) 5/3 also has uniform donor stacks similar to (TTM-TTP)I 3 , and it exhibits metallic conductivity down to T MI = 20 K (see also figure 17).…”

Section: (Ttm-ttp)a Xmentioning

confidence: 99%

Tetrathiapentalene-based organic conductors

Misaki

2009

Science and Technology of Advanced Materials

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The synthesis, structure and properties of tetrathiapentalene-based (TTP) organic conductors are reviewed. Among various TTP-type donors, bis-fused tetrathiafulvalene, 2,5-bis(1,3-dithiol-2-ylidene)-1,3,4,6-tetrathiapentalene (BDT-TTP) and its derivatives afford many metallic radical cation salts stable down to low temperatures, regardless of the size and shape of the counter anions. Most BDT-TTP conductors have a β-type donor arrangement with almost uniform stacks. Introduction of appropriate substituents results in molecular packing that differs from the β-type. A vinylogous TTP, 2-(1,3-dithiol-2-ylidene)-5-(2-ethanediylidene-1,3-dithiole)-1,3,4,6-tetrathiapentalene (DTEDT) has yielded an organic superconductor (DTEDT) 3 Au(CN) 2 as well as metallic radical cation salts, regardless of the counter anions. (Thio)pyran analogs of TTP, namely (T)PDT-TTP and its derivatives produce molecular conductors with novel molecular arrangements. A TTP analog with reduced π-electron system 2,5-bis(1,3-dithian-2-ylidene)-1,3,4,6-tetrathiapentalene (BDA-TTP) has afforded several organic superconductors. Highly conducting molecular metals with unusual oxidation states (+1, +5/3 and neutral) have been developed on the basis of 2,5-bis(1,3-dithiol-2-ylidene)-1,3,4,6-tetrathiapentalene (BDT-TTP) derivatives and analogous metal derivatives M(dt) 2 (M = Ni, Au).

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“…It was expected that the intra-molecular charge distribution of TTM-TTP donor is responsible for the non-magnetic stack dimerization. On the other hand, NMR study 12,13) claimed a "2-0-2-0" type charge ordering state below T MI = 120 K, so that the TTM-TTP 0 and TTM-TTP 2+ molecules are alternately arranged by large V in the stacks. However, our observation suggests that the metallic state is well described by the standard Hubbard model without V .…”

Section: Resultsmentioning

confidence: 99%

Metallization of the Organic Conductor (TTM-TTP)I₃with a Highly One-Dimensional Half-Filled Band under Pressure beyond 7 GPa

et al. 2007

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It is theoretically predicted that the ground state of the one-dimensional (1D) half-filled system is the Mott insulator at any positive on-site Coulomb interaction U . In this paper, we demonstrate that (TTM-TTP)I3 with a highly 1D half-filled energy band is almost metallized by the application of pressure beyond 7 GPa. We find that the metal-insulator transition temperature decreases linearly with increasing pressure and is directing towards 0 K near 10 GPa. Above 5.7 GPa, the metallic behaviors are observed in the high-temperature region for 70 < T < 300 K, in which the temperature dependence of the resistivity is described by ρ(T ) ∝ T α with α ∼ 0.3. The nature of the metallic state is discussed in terms of the Tomonaga-Luttinger liquid described by the Hubbard model. KEYWORDS: (TTM-TTP)I3, organic conductor, one-dimensional system, half-filling, high-pressure, Tomonaga-Luttinger liquid, Hubbard model, Kρ IntroductionMetal-insulator (MI) transitions by Coulomb interaction are accompanied with huge resistance change and are widely observed in strongly correlated systems. Many theories of strongly correlated systems begin with a Hubbard model because of its simplicity.1) The Hubbard model is the prototypical model used for the description of correlated fermions in a variety of materials, ranging from high-T c superconductors to heavy fermion compounds and organic molecular crystals. In spite of its apparent simplicity, there is still no general solution, or even a consensus on its fundamental properties for the Hubbard model. Notable exceptions are the cases of oneand infinite-dimensions.2, 3) In one-dimension, an exact solution is available.4) Especially, the one-dimensional (1D) half-filled case is special but important because it corresponds to the strong coupling limit of the Hubbard model, i.e., U → ∞. 5) That is, no matter how small U is, the ground state is the Mott insulator. Thus metallization of the 1D half-filled system is one of the most challenging problems in the strongly correlated electronic systems.In this paper, we report the metallization of (TTM-TTP)I 3 with a highly 1D half-filled band, 6) where TTM-TTP stands for 2,5-bis[4,5-bis(methylthio)-1,3-dithiol-2-ylidene]-1,3,4,6-tetrathiapentalene [see Fig. 1(a)]. 7,8) In the interchain directions, the TTM-TTP molecules cannot approach close to each other because of the steric hindrance of the terminal -SCH 3 groups.7) According to the band structure calculation, the interchain interactions, t a , t b (< 0.01 eV) are less than 1/20 of the intrachain interaction, t c = 0.26 eV, which is much more onedimensional than the typical quasi-1D Bechgaard salts.

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Electronic state of a new organic conductor (TTM-TTP)I3 with a one-dimensional half-filled band

Cited by 17 publications

References 4 publications

Ab initio derivation of multi-orbital extended Hubbard model for molecular crystals

Ab initio derivation of multi-orbital extended Hubbard model for molecular crystals

Tetrathiapentalene-based organic conductors

Metallization of the Organic Conductor (TTM-TTP)I₃with a Highly One-Dimensional Half-Filled Band under Pressure beyond 7 GPa

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Electronic state of a new organic conductor (TTM-TTP)I3 with a one-dimensional half-filled band

Cited by 17 publications

References 4 publications

Ab initio derivation of multi-orbital extended Hubbard model for molecular crystals

Ab initio derivation of multi-orbital extended Hubbard model for molecular crystals

Tetrathiapentalene-based organic conductors

Metallization of the Organic Conductor (TTM-TTP)I3with a Highly One-Dimensional Half-Filled Band under Pressure beyond 7 GPa

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Metallization of the Organic Conductor (TTM-TTP)I₃with a Highly One-Dimensional Half-Filled Band under Pressure beyond 7 GPa