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Using Raman scattering spectroscopy, we uncover a complex magnetic behavior of \nio, which stands out among magnetic pyrochlores by the lowest temperature of the all-in-all-out (AIAO) Ir moments ordering ($T^\mathrm{N}_{\small\rm{Ir}}=33$~K) and the highest temperature at which AIAO order of rare-earth Nd ions is detected ($T^\mathrm{*}_{\small\rm{Nd}}$=14~K). Our work suggests that in the temperature range between 14~K and 33~K, Nd magnetic moments exhibit characteristic spin ice fluctuations, which indicate a strong enhancement of magnetic interactions between Nd ions. This complex behavior emerges from the interplay of strong spin-orbit coupling, electronic correlations, and geometric frustration on two magnetic pyrochlore sublattices of Nd and Ir ions. The ordering of Ir magnetic moments is accompanied by an appearance of one-magnon Raman modes at 26.3 and 29.6 meV compatible with the AIAO order and of a broad mode at 14 meV, characteristic of the spinon continuum originated from Nd spin ice fluctuations. While two one-magnon excitations show minimal temperature evolution with decreasing temperature, the 14 meV mode shifts to higher frequencies as the temperature approaches a crossover to Nd AIAO order, broadens and disappears below 14~K. An additional two-magnon excitation of the AIAO Nd order at around 33 meV appears in the spectra at low temperatures.

BaCo2(AsO4)2 (BCAO) has seen extensive study since its initial identification as a proximate Kitaev quantum spin liquid candidate. Thought to be described by the highly anisotropic XXZ-J_1-J_3 model, the ease with which magnetic order is suppressed in the system indicates proximity to a spin liquid phase. Upon chemical tuning via partial arsenic substitution with vanadium, we show an initial suppression of long-range incommensurate order in the BCAO system to T = 3.0 K, followed by increased spin freezing at higher substitution levels. Between these two regions, at around 10% substitution, the system is shown to pass through a critical point where the competing J_1/J_3 exchange interactions become more balanced, producing a more complex magnetic ground state, likely stabilized by quantum fluctuations. This state shows how slight compositional change in magnetically-frustrated systems may be leveraged to tune ground state degeneracies and potentially realize a quantum spin liquid state., Main text (43 pages, 9 figures, 1 table); Supplementary information (32 pages, 18 figures, 14 tables)

Mutual interactions in many-body systems bring about a variety of exotic phases, among which liquid-like states failing to order due to frustration are of keen interest. Recently, an organic system with an anisotropic triangular lattice of molecular dimers has been suggested to host a dipole liquid arising from intradimer charge-imbalance instability, possibly offering an unprecedented stage for the spin degrees of freedom. Here we show that an extraordinary unordered(unfrozen) spin state having soft-matter-like spatiotemporal characteristics is substantiated in this system. $^1$H NMR spectra and magnetization measurements indicate that gigantic, staggered moments are non-linearly and inhomogeneously induced by magnetic field whereas the moments vanish in the zero-field limit. The analysis of the NMR relaxation rate signifies that the moments fluctuate at a characteristic frequency slowing down to below MHz at low temperatures. The inhomogeneity, local correlation, and slow dynamics indicative of middle-scale dynamical correlation length suggest a novel frustration-driven spin clusterization., 13 pages, 11 figures, 1 table

Corkite, PbFe3(PO4)(SO4)(OH)6, an understudied relative of the jarosite family of Heisenberg antiferromagnets, has been synthesized and its magnetic properties characterized for the first time. Relative to natural samples, synthetic corkite displays signatures in both infrared and Raman spectra of a more ordered arrangement of polyanion groups about the kagomé sublattice that retains inversion symmetry. Magnetic susceptibility measurements reveal that dried corkite undergoes a transition to a long-range, antiferromagnetically-ordered state below TN = 48 K, lower than that observed in the majority of jarosite phases, and indicative of further spin frustration. Curie-Weiss fitting of the measured magnetic susceptibility yields an effective magnetic moment of peff = 6.29(1) muB/Fe^3+ and theta_CW = -526.0(1.1) K, analogous to that observed in similar high-spin Fe^3+ systems, and indicative of strong antiferromagnetic coupling. Estimation of the change in magnetic entropy as a function of temperature from T = 0 K to T = 195 K, dS_mag = 14.86 J/mol_Fe^3+ K, is also in good agreement with the dS_mag = Rln(2S+1) = 14.9 J/mol K expected for a S = 5/2 system. In comparison to the pure jarosites, where both structure and magnetism remain largely invariant upon a variety of chemical substitutions, the replacement of one sulfate group per formula unit with a higher-valent phosphate group applies additional steric and electronic pressure on the kagomé lattice in corkite, further frustrating the magnetic ground state of the material. Corkite thus represents both an outlier in the known body of jarosite-type materials, and an illustration of how existing structures may be further strained in the development of highly frustrated magnetic systems., 27 pages, 5 figures, 4 tables

Magnetic materials with pyrochlore crystal structure form exotic magnetic states due to the high lattice frustration. In this work we follow the effects of coupling of the lattice and electronic and magnetic degrees of freedom in two Praseodymium-based pyrochlores Pr$_2$Zr$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$. In both materials the presence of magnetic interactions does not lead to magnetically ordered low temperature states, however their electronic properties are different. A comparison of Raman phonon spectra of Pr$_2$Zr$_2$O$_7$ and Pr$_2$Ir$_2$O$_7$ allows us to identify magneto-elastic coupling in Pr$_2$Zr$_2$O$_7$ that elucidates its magnetic properties at intermediate temperatures, and allows us to characterize phonon-electron coupling in the semimetallic Pr$_2$Ir$_2$O$_7$. We also show that the effects of random disorder on the Raman phonon spectra is small., 6 pages, 5 figures

Pr$_2$Zr$_2$O$_7$ is a pyrochlore quantum spin-ice candidate. Using Raman scattering spectroscopy we probe crystal electric field excitations of Pr$^{3+}$, and demonstrate the importance of their interactions with the lattice. We identify a vibronic interaction with a phonon that leads to a splitting of a doublet crystal field excitation at around 55~meV. We also probe a splitting of the non-Kramers ground state doublet of Pr$^{3+}$ by observing a double line of the excitations to the first excited singlet state $E^0_g \rightarrow A_{1g}$. We show that the splitting has a strong temperature dependence, with the doublet structure most prominent between 50~K and 100~K, and the weight of one of the components strongly decreases on cooling. We suggest a static or dynamic deviation of Pr$^{3+}$ from the position in the ideal crystal structure can be the origin of the effect, with the deviation strongly decreasing at low temperatures., 6 pages, 3 figures

NiGa$_2$S$_4$ is a triangular lattice S=1 system with strong two-dimensionality of the lattice, actively discussed as a candidate to host spin-nematic order brought about by strong quadrupole coupling. Using Raman scattering spectroscopy we identify a phonon of E$_g$ symmetry which can modulate magnetic exchange $J_1$ and produce quadrupole coupling. Additionally, our Raman scattering results demonstrate a loss of local inversion symmetry on cooling, which we associate with sulfur vacancies. This will lead to disordered Dzyaloshinskii-Moriya interactions, which can prevent long range magnetic order. Using magnetic Raman scattering response we identify 160~K as a temperature of an upturn of magnetic correlations. The temperature below 160~K, but above 50~K where antiferromagnetic magnetic start to increase, is a candidate for spin-nematic regime.

We perform magnetic susceptibility and magnetic torque measurements on the organic $��$-(BEDT-TTF)$_2$Hg(SCN)$_2$Br, which is recently suggested to host an exotic quantum dipole-liquid in its low-temperature insulating phase. Below the metal-insulator transition temperature, the magnetic susceptibility follows a Curie-Weiss law with a positive Curie-Weiss temperature, and a particular $M\propto \sqrt{H}$ curve is observed. The emergent ferromagnetically interacting spins amount to about 1/6 of the full spin moment of localized charges. Taking account of the possible inhomogeneous quasi-charge-order that forms a dipole-liquid, we construct a model of antiferromagnetically interacting spin chains in two adjacent charge-ordered domains, which are coupled via fluctuating charges on a Mott-dimer at the boundary. We find that the charge fluctuations can draw a weak ferromagnetic moment out of the spin singlet domains., 9 pages, 5 figures, Supplementary Material attached

Strong electronic interactions can drive a system into a state with a symmetry breaking. Lattice frustration or competing interactions tend to prevent a symmetry breaking, leading to quantum disordered phases. In spin systems frustration can produce a spin liquid state. Frustration of a charge degree of freedom also can result in various exotic states, however, experimental data on these effects is scarce. In this work we demonstrate how a charge ordered ferroelectric looses the order on cooling to low temperatures using an example of a Mott insulator on a weakly anisotropic triangular lattice $\kappa$-(BEDT-TTF)$_2$Hg(SCN)$_2$Cl. Typically, a low temperature ordered state is a ground state of a system, and the demonstrated re-entrant behavior is unique. Raman scattering spectroscopy finds that this material enters an insulating ferroelectric `dipole solid' state at $T=30~K$, but below $T=15~K$ the order melts, while preserving the insulating energy gap. The resulting phase diagram is relevant to other quantum paraelectric materials.

Using Raman spectroscopy, we investigate the lattice phonons, magnetic excitations, and magneto-elastic coupling in the distorted triangular-lattice Heisenberg antiferromagnet alpha-SrCr2O4, which develops helical magnetic order below 43 K. Temperature dependent phonon spectra are compared to predictions from density functional theory calculations which allows us to assign the observed modes and identify weak effects arising from coupled lattice and magnetic degrees of freedom. Raman scattering associated with two-magnon excitations is observed at 20 meV and 40 meV. These energies are in general agreement with our ab-initio calculations of exchange interactions and earlier theoretical predictions of the two-magnon Raman response of triangular-lattice antiferromagnets. The temperature dependence of the two-magnon excitations indicates that spin correlations persist well above the N\'eel temperature.

KNi$_2$Se$_2$ exhibits an increase of symmetry on cooling below $T\le50$ K, as observed by Raman spectroscopy and synchrotron x-ray diffraction. X-ray absorption spectroscopy confirms that the symmetry increase is due to changes in nickel-nickel interactions and suppression of charge density wave fluctuations. Density functional theory calculations reveal a zone- boundary lattice instability that provides a model of the room-temperature x-ray pair distribution function data, but fails to describe the higher local symmetry observed for $T\le50$K. Together, these results support many- body correlation effects as drivers for the unusual heavy fermion electronic ground state in KNi$_2$Se$_2$., Comment: 4 figures

We report on the anisotropic response, the charge and lattice dynamics of normal and charge-ordered phases with horizontal stripes in single crystals of the organic conductor alpha-(BEDT-TTF)2I3 determined by dc resistivity, dielectric and optical spectroscopy. An overdamped Drude response and a small conductivity anisotropy observed in optics is consistent with a weakly temperature dependent dc conductivity and anisotropy at high temperatures. The splitting of the molecular vibrations nu27(Bu) evidences the abrupt onset of static charge order below TCO=136 K. The drop of optical conductivity measured within the ab plane of the crystal is characterized by an isotropic gap that opens of approximately 75 meV with several phonons becoming pronounced below. Conversely, the dc conductivity anisotropy rises steeply, attaining at 50 K a value 25 times larger than at high temperatures. The dielectric response within this plane reveals two broad relaxation modes of strength Deltaepsilon_LD ~= 5000 and Deltaepsilon_SD ~= 400, centered at 1 kHz < f_LD < 100 MHz and f_SD ~= 1 MHz. The anisotropy of the large-mode (LD) mean relaxation time closely follows the temperature behavior of the respective dc conductivity ratio. We argue that this phason-like excitation is best described as a long-wavelength excitation of a 2kF bond-charge density wave expected theoretically for layered quarter-filled electronic systems with horizontal stripes. Conversely, based on the theoretically expected ferroelectric-like nature of the charge-ordered phase, we associate the small-mode (SD) relaxation with the motion of domain-wall pairs, created at the interface between two types of domains, along the a and b axes. We also consider other possible theoretical interpretations and discuss their limitations., 13 pages, 16 figures, resubmitted to Phys. Rev. B

The charge response of charge-ordered state in the organic conductor alpha-(BEDT-TTF)2I3 is characterized by dc resistivity, dielectric and optical spectroscopy in different crystallographic directions within the two-dimensional conduction layer. Two dielectric modes are detected. The large mode is related to the phason-like excitation of the 2kF bond-charge density wave which forms in the ab plane. The small dielectric mode is associated with the motion of domain-wall pairs along the a- and b-axes between two types of domains which are created due to inversion symmetry breaking., resubmitted to Phys. Rev. Lett.; 4 pages, 3 figures

Infrared reflection measurements of the half-filled two-dimensional organic conductors $��$-(BEDT-TTF)$_2$Cu[N(CN)$_{2}$]Br$_{x}$Cl$_{1-x}$ were performed as a function of temperature ($5 {\rm K}, 12 pages, 12 figures