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Melanins are pigmentary macromolecules found throughout the biosphere that, in the 1970s, were discovered to conduct electricity and display bistable switching. Since then, it has been widely believed that melanins are naturally occurring amorphous organic semiconductors. Here, we report electrical conductivity, muon spin relaxation, and electron paramagnetic resonance measurements of melanin as the environmental humidity is varied. We show that hydration of melanin shifts the comproportionation equilibrium so as to dope electrons and protons into the system. This equilibrium defines the relative proportions of hydroxyquinone, semiquinone, and quinone species in the macromolecule. As such, the mechanism explains why melanin at neutral pH only conducts when \"wet\" and suggests that both carriers play a role in the conductivity. Understanding that melanin is an electronic-ionic hybrid conductor rather than an amorphous organic semiconductor opens exciting possibilities for bioelectronic applications such as ion-toelectron transduction given its biocompatibility.

Quantum materials exhibiting magnetic frustration are connected to diverse phenomena, including high Tc superconductivity, topological order, and quantum spin liquids (QSLs). A QSL is a quantum phase (QP) related to a quantum-entangled fluid-like state of matter. Previous experiments on QSL candidate materials are usually interpreted in terms of a single QP, although theories indicate that many distinct QPs are closely competing in typical frustrated spin models. Here we report on combined temperature-dependent muon spin relaxation and specific heat measurements for the triangular-lattice QSL candidate material 1T-TaS2 that provide evidence for competing QPs. The measured properties are assigned to arrays of individual QSL layers within the layered charge density wave structure of 1T-TaS2 and their characteristic parameters can be interpreted as those of distinct Z2 QSL phases. The present results reveal that a QSL description can extend beyond the lowest temperatures, offering an additional perspective in the search for such materials.

Strong quantum zero-point motion (ZPM) of light nuclei and other particles is a crucial aspect of many state-of-the-art quantum materials. However, it has only recently begun to be explored from an ab initio perspective, through several competing approximations. Here we develop a unified description of muon and light nucleus ZPM and establish the regimes of anharmonicity and positional quantum entanglement where different approximation schemes apply. Via density functional theory and path-integral molecular dynamics simulations we demonstrate that in solid nitrogen, α –N 2 , muon ZPM is both strongly anharmonic and many-body in character, with the muon forming an extended electric-dipole polaron around a central, quantum-entangled [N 2 – μ –N 2 ] + complex. By combining this quantitative description of quantum muon ZPM with precision muon quadrupolar level-crossing resonance experiments, we independently determine the static 14 N nuclear quadrupolar coupling constant of pristine α –N 2 to be –5.36(2) MHz, a significant improvement in accuracy over the previously-accepted value of –5.39(5) MHz, and a validation of our unified description of light-particle ZPM. Quantum entanglement and uncertainty in the positions of light nuclei and implanted particles can crucially impact our understanding of advanced materials. This paper develops a unified theoretical description of these effects and applies it to muon spectroscopy measurements of a material constant to significantly improve their accuracy.

The interplay between magnetism and charge transport is central to understanding colossal magnetoresistance (CMR), a phenomenon well studied in ferromagnets. Recently, antiferromagnetic (AFM) EuCd 2 P 2 has attracted considerable interest due to its remarkable CMR, for which magnetic fluctuations and the formation of ferromagnetic clusters have been proposed as key mechanisms. Here we provide direct evidence that these effects originate from the formation and percolation of magnetic polarons. We employ a complementary set of sensitive probes that allows for a direct comparison of electronic and magnetic properties on multiple time scales revealing pronounced electronic and magnetic phase separation below T * ≈ 2 T N . These measurements indicate an inhomogeneous, percolating electronic system below T * and well above the magnetic ordering temperature T N = 11 K. In applied magnetic fields, the onset of the pronounced negative MR in the paramagnetic regime emerges at a universal critical magnetization. The characteristic size of the magnetic polarons near the percolation threshold is estimated to be ~6−10 nm. Our results establish dynamic polaron percolation within an AFM matrix as the microscopic origin of CMR in EuCd 2 P 2 , providing a unified framework for magnetotransport in Eu-based correlated semiconductors.

The molecular cluster system [Fe19(metheidi)10(OH)14O6(H2O)12]NO3·24H2O, abbreviated as Fe19, contains nineteen Fe(III) ions arranged in a disc-like structure with the total spin S = 35/2. For the first order, it behaves magnetically as a single molecule magnet with a 16 K anisotropy barrier. The high spin value enhances weak intermolecular interactions for both dipolar and superexchange mechanisms and an eventual transition to antiferromagnetic order occurs at 1.2 K. We used neutron diffraction to determine both the mode of ordering and the easy spin axis. The observed ordering was not consistent with a purely dipolar driven order, indicating a significant contribution from intermolecular superexchange. The easy axis is close to the molecular Fe1–Fe10 axis. Inelastic neutron scattering was used to follow the magnetic order parameter and to measure the magnetic excitations. Direct transitions to at least three excited states were found in the 2 to 3 meV region. Measurements below 0.2 meV revealed two low energy excited states, which were assigned to S = 39/2 and S = 31/2 spin states with respective excitation gaps of 1.5 and 3 K. Exchange interactions operating over distances of order 10 Å were determined to be on the order of 5 mK and were eight-times stronger than the dipolar coupling.

The achiral organic radical dinitrophenyl nitronyl nitroxide crystallizes in two enantiomorphs, both being chiral tetragonal space groups that are mirror images of each other. Muon-spin rotation experiments have been performed to study the magnetic properties of these crystals and demonstrate that long-range magnetic order is established below a temperature of 1.10(1) K. Two oscillatory components are detected in the muon data, which show two different temperature dependences.

The precipitate microstructure and vacancy distribution in Al-Mg-Si alloys with different amounts of solute and different heat treatments were investigated by transmission electron microscopy and muon spin relaxation measurements. A high amount of vacancies is normally present in Al-Mg-Si alloys as these bind to atomic clusters. We observe these vacancies to leave the material not before over-aging at very high temperatures such as 623 K (350 °C), meaning that vacancies do not bind to incoherent over-aged precipitates. For samples only stored at room temperature after solution heat treatment, a reduction of muon trapping was found at a temperature of 140 K (−133 °C) when reducing the amount of solute in the alloy. This might be connected to a lower number density of Cluster (1), which contrary to Cluster (2) do not nucleate precipitates upon further aging of the material.

As with quantum spin liquids based on two-dimensional triangular and kagome lattices, the two-dimensional honeycomb lattice with either a strong spin-orbital coupling or a frustrating second-nearest-neighbor coupling is expected to be a source of candidate quantum spin liquids. An ammonium salt [(C 3 H 7 ) 3 NH] 2 [Cu 2 (C 2 O 4 ) 3 ](H 2 O) 2.2 containing hexagonal layers of Cu 2+ was obtained from solution. No structural transition or long-range magnetic ordering was observed from 290 K to 2 K from single crystal X-ray diffraction, specific heat and susceptibility measurements. The anionic layers are separated by sheets of ammonium and H 2 O with distance of 3.5 Å and no significant interaction between anionic layers. The two-dimensional honeycomb lattice is constructed from Jahn-Teller distorted Cu 2+ and oxalate anions, showing a strong antiferromagnetic interaction between S = 1/2 metal atoms with θ = −120 (1) K. Orbital analysis of the Cu 2+ interactions through the oxalate-bridges suggests a stripe mode pattern of coupling with weak ferromagnetic interaction along the b axis and strong antiferromagnetic interaction along the a axis. Analysis of the magnetic susceptibility shows that it is dominated by a quasi-one-dimensional contribution with spin chains that are at least as well isolated as those of well-known quasi-one-dimensional spin liquids.

Strong hydrogen bonds such as F···H···F offer new strategies to fabricate molecular architectures exhibiting novel structures and properties. Along these lines and, to potentially realize hydrogen-bond mediated superexchange interactions in a frustrated material, we synthesized [H 2 F] 2 [Ni 3 F 6 (Fpy) 12 ][SbF 6 ] 2 (Fpy = 3-fluoropyridine). It was found that positionally-disordered H 2 F + ions link neutral NiF 2 (Fpy) 4 moieties into a kagome lattice with perfect 3-fold rotational symmetry. Detailed magnetic investigations combined with density-functional theory (DFT) revealed weak antiferromagnetic interactions ( J ~ 0.4 K) and a large positive- D of 8.3 K with m s = 0 lying below m s = ±1. The observed weak magnetic coupling is attributed to bond-disorder of the H 2 F + ions which leads to disrupted Ni-F···H-F-H···F-Ni exchange pathways. Despite this result, we argue that networks such as this may be a way forward in designing tunable materials with varying degrees of frustration.

The interplay between magnetism and charge transport is central to understanding colossal magnetoresistance (CMR), a phenomenon well studied in ferromagnets. Recently, antiferromagnetic (AFM) EuCd P has attracted considerable interest due to its remarkable CMR, for which magnetic fluctuations and the formation of ferromagnetic clusters have been proposed as key mechanisms. Here we provide direct evidence that these effects originate from the formation and percolation of magnetic polarons. We employ a complementary set of sensitive probes that allows for a direct comparison of electronic and magnetic properties on multiple time scales revealing pronounced electronic and magnetic phase separation below ≈ 2 . These measurements indicate an inhomogeneous, percolating electronic system below and well above the magnetic ordering temperature = 11 K. In applied magnetic fields, the onset of the pronounced negative MR in the paramagnetic regime emerges at a universal critical magnetization. The characteristic size of the magnetic polarons near the percolation threshold is estimated to be ~6-10 nm. Our results establish dynamic polaron percolation within an AFM matrix as the microscopic origin of CMR in EuCd P , providing a unified framework for magnetotransport in Eu-based correlated semiconductors.