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Flat bands that do not merely arise from weak interactions can produce exotic physical properties, such as superconductivity or correlated many-body effects. The quantum metric can differentiate whether flat bands will result in correlated physics or are merely dangling bonds. A potential avenue for achieving correlated flat bands involves leveraging geometrical constraints within specific lattice structures, such as the kagome lattice; however, materials are often more complex. In these cases, quantum geometry becomes a powerful indicator of the nature of bands with small dispersions. We present a simple, soft-chemical processing route to access a flat band with an extended quantum metric below the Fermi level. By oxidizing Ni-kagome material Cs2Ni3S4to CsNi3S4, we see a two orders of magnitude drop in the room temperature resistance. However, CsNi3S4is still insulating, with no evidence of a phase transition. Using experimental data, density functional theory calculations, and symmetry analysis, our results suggest the emergence of a correlated insulating state of unknown origin.more » « less
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Optical spectroscopy of quantum materials at ultralow temperatures is rarely explored, yet it may provide critical characterizations of quantum phases not possible using other approaches. We describe the development of a novel experimental platform that enables optical spectroscopic studies, together with standard electronic transport, of materials at millikelvin temperatures inside a dilution refrigerator. The instrument is capable of measuring both bulk crystals and micrometer-sized two-dimensional van der Waals materials and devices. We demonstrate its performance by implementing photocurrent-based Fourier transform infrared spectroscopy on a monolayer WTe2 device and a multilayer 1T-TaS2 crystal, with a spectral range available from the near-infrared to the terahertz regime and in magnetic fields up to 5 T. In the far-infrared regime, we achieve spectroscopic measurements at a base temperature as low as ∼43 mK and a sample electron temperature of ∼450 mK. Possible experiments and potential future upgrades of this versatile instrumental platform are envisioned.more » « less
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Subchalcogenides are uncommon, and their chemical bonding results from an interplay between metal–metal and metal–chalcogenide interactions. Herein, we present Ir 6 In 32 S 21 , a novel semiconducting subchalcogenide compound that crystallizes in a new structure type in the polar P 31 m space group, with unit cell parameters a = 13.9378(12) Å, c = 8.2316(8) Å, α = β = 90°, γ = 120°. The compound has a large band gap of 1.48(2) eV, and photoemission and Kelvin probe measurements corroborate this semiconducting behavior with a valence band maximum (VBM) of −4.95(5) eV, conduction band minimum of −3.47(5) eV, and a photoresponse shift of the Fermi level by ∼0.2 eV in the presence of white light. X-ray absorption spectroscopy shows absorption edges for In and Ir do not indicate clear oxidation states, suggesting that the numerous coordination environments of Ir 6 In 32 S 21 make such assignments ambiguous. Electronic structure calculations confirm the semiconducting character with a nearly direct band gap, and electron localization function (ELF) analysis suggests that the origin of the gap is the result of electron transfer from the In atoms to the S 3p and Ir 5d orbitals. DFT calculations indicate that the average hole effective masses near the VBM (1.19 m e ) are substantially smaller than the average electron masses near the CBM (2.51 m e ), an unusual feature for most semiconductors. The crystal and electronic structure of Ir 6 In 32 S 21 , along with spectroscopic data, suggest that it is neither a true intermetallic nor a classical semiconductor, but somewhere in between those two extremes.more » « less
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