Unconventional Magnetic and Resistive Hysteresis in an Iodine‐Bonded Molecular Conductor

Kawaguchi, Genta; Maesato, Mitsuhiko; Komatsu, Tokutaro; Kitagawa, Hiroshi; Imakubo, Tatsuro; Kiswandhi, Andhika; Graf, David; Brooks, J. S.

doi:10.1002/anie.201503824

Cited by 6 publications

(22 citation statements)

References 38 publications

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“…Remarkably, we observed a large shift in the spin-flop field of d -spins at low temperatures below about 1.3 K in (DIETSe) 2 FeBr 2 Cl 2 , which resulted in large hysteresis in both MR and magnetization. 21 On the other hand, in the pristine FeX 4 [X = Br, Cl] salts, the hysteresis of the spin-flop field is negligibly small. [18][19][20][21] These differences are attributable in part to the random exchange in the FeBr 2 Cl 2 salt.…”

Section: Saltsmentioning

confidence: 99%

“…21 On the other hand, in the pristine FeX 4 [X = Br, Cl] salts, the hysteresis of the spin-flop field is negligibly small. [18][19][20][21] These differences are attributable in part to the random exchange in the FeBr 2 Cl 2 salt. The randomly substituted halogens in magnetic anions give rise to locally different exchange fields, leading to the hysteretic response to the external magnetic field.…”

Section: Saltsmentioning

confidence: 99%

“…Indeed, some Q1D π-d conductors exhibit anomalous magnetoresistance (MR) associated with reconfiguration of antiferromagnetic (AF) d -spins, indicating the interplay between the local moments and itinerant electrons. [12][13][14][15][16][17][18][19][20][21] The coexistence of SDW and 3d local moments has been studied in (DIETSe) 2 FeCl 4 , where DIETSe represents diiodo(ethylenedithio)tetraselenafulvalene ( Fig. 1(a)).…”

Section: Introductionmentioning

confidence: 99%

“…18,19 The nesting instability of Q1D Fermi surfaces can be suppressed by substituting Cl with Br. (DIETSe) 2 GaBr 4 shows normal metallic behavior down to 2 K, whereas (DIETSe) 2 FeBr 4 undergoes an M-I transition induced by AF ordering of d -spins at 7 K. 17,21 It suggests that the Ruderman-Kittel-Kasuya-Yosida (RKKY)-type interaction [23][24][25] with SDW instability plays an important role in the FeBr 4 salt. The higher Néel temperature T N of the FeBr 4 salt indicates stronger π-d interactions than in the FeCl 4 salt.…”

Section: Introductionmentioning

confidence: 99%

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Interplay between spin-density wave and 3d local moments with random exchange in a molecular conductor

et al. 2016

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We present the results of high-pressure transport measurements on the anion-mixed molecular conductors (DIETSe)2MBr2Cl2 [DIETSe = diiodo(ethylenedithio)tetraselenafulvalene; M = Fe, Ga]. They undergo a metal-insulator (M-I) transition below 9 K at ambient pressure, which is suppressed by applying pressure, indicating a spin-density-wave (SDW) transition caused by a nesting instability of the quasi-one-dimensional (Q1D) Fermi surface, as observed in the parent compounds (DIETSe)2MCl4 [M = Fe, Ga]. In the metallic state, the existence of the Q1D Fermi surface is confirmed by observing the Lebed resonance. The critical pressures of the SDW, Pc, of the MBr2Cl2 [M = Fe, Ga] salts are significantly lower than those of the the MCl4 [M = Fe, Ga] salts, suggesting chemical pressure effects. Above Pc, field-induced SDW transitions appear, as evidenced by kink structures in the magnetoresistance (MR) in both salts. The FeBr2Cl2 salt also shows antiferromagnetic (AF) ordering of d-spins at 4 K, below which significant spin-charge coupling is observed. A large positive MR change up to 150% appears above the spin-flop field at high pressure. At low pressure, in particular below Pc, a dip or kink structure appears in MR at the spin-flop field, which shows unconventionally large hysteresis at low temperature (T < 1 K). The hysteresis region clearly decreases with increasing pressure towards Pc, strongly indicating that the coexisting SDW plays an important role in the enhancement of magnetic hysteresis besides the random exchange interaction.

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Section: Saltsmentioning

confidence: 99%

Section: Saltsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Interplay between spin-density wave and 3d local moments with random exchange in a molecular conductor

et al. 2016

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“…[11] Thec rystal structures of 1 and 2 are isostructural to the pristine (DIETSe) 2 MX 4 [M = Fe,Ga; X= Br,Cl] (Figure 1c; Figures S1 and S2). [6,12] DIETSe molecules uniformly stack parallel to the a-axis in ah ead-to-tail manner,g iving rise to the highest conductivity along the a-axis direction. Figure 1d shows short I···X [X = Br, Cl] contacts between DIETSe and anion, which are shorter than the sum of the van der Waals radii:I···Cl = 3.73 , I···Br = 3.83 , indicating that the iodine bonds play an important role in stabilizing the structure.…”

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Unconventional Magnetic and Resistive Hysteresis in an Iodine‐Bonded Molecular Conductor

et al. 2015

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Simultaneous manipulation of both spin and charge is acrucial issue in magnetic conductors.Wereport on astrong correlation between magnetism and conductivity in the iodinebonded molecular conductor (DIETSe) 2 FeBr 2 Cl 2 [DIETSe = diiodo(ethylenedithio)tetraselenafulvalene],w hichi st he first molecular conductor showing al arge hysteresis in both magnetic moment and magnetoresistance associated with as pin-flop transition. Utilizing am ixed-anion approach and iodine bonding interactions,wetailored amolecular conductor with random exchange interactions exhibiting unforeseen physical properties.

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Use of Halogen Bonding in a Molecular Solid Solution to Simultaneously Control Spin and Charge

et al. 2016

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Halogen-bonding interactions have attracted increasing attention in various fields of molecular science. Here we report the first comprehensive study of halogen-bonding-utilized solid solution for simultaneous control of multifunctional properties. A series of anion-mixed molecular conductors (DIE-TSe) 2 MBr 4x Cl 4(1−x) [DIETSe = diiodo(ethylenedithio)tetraselenafulvalene; M = Fe, Ga; 0 < x < 1] were synthesized without changing crystal structure utilizing strong halogen bonds between DIETSe molecules and anions. Detailed physical property measurements (T > 0.3 K, H < 35 T) using the single crystals demonstrated simultaneous control of both spin and charge degrees of freedom. The increase in Br content x gradually suppresses a metal−insulator transition attributed to the nesting instability of the quasi-one-dimensional Fermi surfaces. It suggests the dimensionality of π electrons is extended by increasing the anion size, which is opposite of the typical effect of chemical pressure. We found that the "negative" chemical pressure is associated with the characteristic halogen-bonding network. Br substitution also enhances the antiferromagnetic (AF) ordering of d-electron spins in the Fe salts, as indicated by the Neél temperature, AF phase boundary field, and saturation field. Furthermore, we observed hysteresis in both magnetization and resistivity only in halogen-mixed salts at very low temperatures, indicating simultaneous spin and charge manipulation by alloying.

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Unconventional Magnetic and Resistive Hysteresis in an Iodine‐Bonded Molecular Conductor

Cited by 6 publications

References 38 publications

Interplay between spin-density wave and 3d local moments with random exchange in a molecular conductor

Interplay between spin-density wave and 3d local moments with random exchange in a molecular conductor

Unconventional Magnetic and Resistive Hysteresis in an Iodine‐Bonded Molecular Conductor

Use of Halogen Bonding in a Molecular Solid Solution to Simultaneously Control Spin and Charge

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