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α-RuCl3 is considered to be the top candidate material for the experimental realization of the celebrated Kitaev model, where ground states are quantum spin liquids with interesting fractionalized excitations. It is, however, known that additional interactions beyond the Kitaev model trigger in α-RuCl3 a long-range zigzag antiferromagnetic ground state. In this work, we investigate a nanoflake of α-RuCl3 through guarded high impedance measurements aimed at reaching the regime where the system turns into a zigzag antiferromagnet. We investigated a variety of temperatures (1.45–175 K) and out-of-plane magnetic fields (up to 11 T), finding a clear signature of a structural phase transition at ≈160 K as reported for thin crystals of α-RuCl3, as well as a thermally activated behavior at temperatures above ≈30 K, with a characteristic activation energy significantly smaller than the energy gap that we observe for α-RuCl3 bulk crystals through our angle resolved photoemission spectroscopy (ARPES) experiments. Additionally, we found that below ≈30 K, transport is ruled by Efros–Shklovskii variable range hopping (VRH). Most importantly, our data show that below the magnetic ordering transition known for bulk α-RuCl3 in the frame of the Kitaev–Heisenberg model (≈7 K), there is a clear deviation from VRH or thermal activation transport mechanisms. Our work demonstrates the possibility of reaching, through specialized high impedance measurements, the thrilling ground states predicted for α-RuCl3 at low temperatures in the frame of the Kitaev–Heisenberg model and informs about the transport mechanisms in this material in a wide temperature range.
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Liquid-Phase Exfoliation of Magnetically and Optoelectronically Active Ruthenium Trichloride Nanosheets
α-RuCl3 is a layered transition metal halide that possesses a range of exotic magnetic, optical, and electronic properties including fractional excitations indicative of a proximate Kitaev quantum spin liquid (QSL). While previous reports have explored these properties on idealized single crystals or mechanically exfoliated samples, the scalable production of α-RuCl3 nanosheets has not yet been demonstrated. Here, we perform liquid-phase exfoliation (LPE) of α-RuCl3 through an electrochemically assisted approach, which yields ultrathin, electron-doped α-RuCl3 nanosheets that are then assembled into electrically conductive large-area thin films. The crystalline integrity of the α-RuCl3 nanosheets following LPE is confirmed through a wide range of structural and chemical analyses. Moreover, the physical properties of the LPE α-RuCl3 nanosheets are investigated through electrical, optical, and magnetic characterization methods, which reveal a structural phase transition at 230 K that is consistent with the onset of Kitaev paramagnetism in addition to an antiferromagnetic transition at 2.6 K. Intercalated ions from the electrochemical LPE protocol favorably alter the optical response of the α-RuCl3 nanosheets, enabling large-area Mott insulator photodetectors that operate at telecommunications-relevant infrared wavelengths near 1.55 μm. These photodetectors show a linear photocurrent response as a function of incident power, which suggests negligible trap-mediated recombination or photothermal effects, ultimately resulting in a photoresponsivity of ≈2 mA/W.
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- Award ID(s):
- 2004420
- PAR ID:
- 10334666
- Date Published:
- Journal Name:
- ACS Nano
- ISSN:
- 1936-0851
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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We study the nature of the debated thermal Hall effect in the candidate Kitaev material α-RuCl3. Without assuming the existence of a gapped spin liquid, we show that a realistic minimal spin model in the canted zigzag phase suffices, at the level of linear spin-wave theory, to qualitatively explain the observed temperature and magnetic field dependence of the non-quantized thermal Hall conductivity κ_xy, with its origin lying in the Berry curvature of the magnon bands. The magnitude of the effect is however too small compared to the measurement by Czajka et al. [Nat. Mater. 22, 36-41 (2023)], even after scanning a broad range of model parameters so as to maximize κ_xy/T. Recent experiments suggest that phonons play an important role, which we show couple to the spins, endowing phonons with chirality. The resulting intrinsic contribution, from both magnons and phonons, is however still insufficient to explain the observed magnitude of the Hall signal. After careful analysis of the extrinsic phonon mechanisms, we use the recent experimental data on thermal transport in α-RuCl3 by Lefrançois et al. [Phys. Rev. X 12, 021025 (2022)] to determine the phenomenological ratio of the extrinsic and intrinsic contributions η≡κ_E/κ_I. We find η=1.2±0.5, which when combined with our computed intrinsic value, explains quantitavely both the magnitude and detailed temperature dependence of the experimental thermal Hall effect in α-RuCl3.more » « less
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We report liquid-phase exfoliation (LPE) of bulk layered-structure semiconductor, MnIn 2 Se 4 , to nanoscale thick sheets by ultrasonication followed by sequential centrifugation at 2000, 5000, and 7500 rpm. The nanosheets exfoliated by LPE in isopropyl alcohol show an average thickness of 50, 40, and 14 nm, respectively. The smallest of these values corresponds approximately to ten 7-atom thick [Se–In–Se–Mn–Se–In–Se] layers that compose the bulk structure of MnIn 2 Se 4 . Both the bulk material and the exfoliated samples show photoluminescence, but the weak shoulder observed from the indirect band gap emission is obviously suppressed in the nanosheet samples as compared to the bulk sample. Similar to the bulk, the nanosheets isolated at 2000 and 5000 rpm exhibit spin-glass behavior with a freezing temperature of ∼3 K. In contrast, the nanosheets isolated at 7500 rpm do not exhibit any anomalies in their low-temperature magnetic behavior. These results demonstrate the possibility to extend the LPE technique to van-der-Waals materials with several-atom-thick layers.more » « less
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The leading order nonlinear (NL) susceptibility, χ3, in a paramagnet is negative and diverges as T → 0. This divergence is destroyed when spins correlate and the NL response provides unique insights into magnetic order. Dimensionality, exchange interaction, and preponderance of quantum effects all imprint their signatures in the NL magnetic response. Here, we study the NL susceptibilities in the proximate Kitaev magnet α-RuCl3, which differs from the expected antiferromagnetic behavior. For T < Tc = 7.5 K and field B in the ab-plane, we obtain contrasting NL responses in low (<2 T) and high field regions. For low fields, the NL behavior is dominated by a quadratic response (positive χ2), which shows a rapid rise below Tc. This large χ2 > 0 implies a broken sublattice symmetry of magnetic order at low temperatures. Classical Monte Carlo (CMC) simulations in the standard K − H − Γ model secure such a quadratic B dependence of M, only for T ≈ Tc with χ2 being zero as T → 0. It is also zero for all temperatures in exact diagonalization calculations. On the other hand, we find an exclusive cubic term (χ3) that describes the high field NL behavior well. χ3 is large and positive both below and above Tc crossing zero only for T > 50 K. In contrast, for B ∥ c-axis, no separate low/high field behaviors are measured and only a much smaller χ3 is apparent.more » « less
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1021/acsnano.2c04888
