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The intricate interplay between spin and lattice degrees of freedom in two-dimensional magnetic materials plays a pivotal role in modifying their magnetic characteristics, engendering hybrid quasiparticles, and implementing functional devices. Herein, we present our comprehensive and in-depth investigations on magnetic and lattice excitations of MnPSe3-xSx (x = 0, 0.5, and 1.5) alloys, utilizing temperature- and polarization-dependent Raman scattering. Our experimental results reveal the occurrence of multiple phase transitions, evidenced by notable changes in phonon self-energy and the appearance or splitting of phonon modes. These emergent phases are tied to the development of long and short-range spin-spin correlations, as well as to spin reorientations or magnetic instabilities. Our analysis of two-magnon excitations as a function of temperature and composition showcases their hybridization with phonons whose degree weakens with increasing x. Moreover, the suppression of spin-dependent phonon intensity in chemically most-disordered MnPSe3-xSx (x = 1.5) suggests that chalcogen substitution offers a control knob of tuning spin and phonon dynamics by modulating concurrently superexchange pathways and a degree of trigonal distortions.

Phase transitions with lowering temperature is a manifestation of decreased entropy and within the Landau theoretical framework these are accompanied by the symmetry breaking. Whenever a symmetry is broken weakly or strongly, it leaves its trail and the same may be captured indirectly using renormalization of the quasi-particle excitations. Cr2Ge2Te6, a quasi-two-dimensional magnetic material, provides a rich playground to probe dynamics of the quasi-particle excitations as well as multiple phase transitions with lowering temperature intimately linked with the lattice and spin degrees of freedom. Here, we report in-depth inelastic light scattering measurements on single crystals of Cr2Ge2Te6 as a function of temperature, from 6 K to 330 K, and polarization. Our measurements reveal the long as well as short range ordering of the spins below Tc (~ 60 K) and T* (~ 180 K), respectively; setting the stage for broken rotational and time reversal symmetry, gauged via the distinct renormalization of the phonon self-energy parameters along with the modes intensity. Our measurements also uncovered an intriguing dependence of the interaction strength between discrete state (phonon here) and the underlying continuum, quantified using the Fano asymmetry parameter, as a function of the scattered light polarization. Our results suggest the possibility of tuning the interaction strength using controlled scattered light and symmetry in this 2D magnet.

Resonance Raman scattering, a very effective and sensitive technique for atomically thin semiconducting transition metal dichalcogenide, can be used to observe the phonons from the entire Brillouin zone. In addition to the significance of resonance effect on the Raman spectrum it may also be used to probe the electron-phonon coupling. Our study is devoted to understand the phonons in layered MoS2, especially for very low frequency range (i.e. below 100 cm-1), as a function of temperature under the resonance effect. Understanding the phonon-phonon and electron-phonon coupling and the effects of temperature on the Raman spectrum are the central points of the present study. We observe the anomalous softening and broadening of a very low frequency phonon mode P3 (~34 cm-1) at low temperature ( i.e below 150 K). We attributed the observed anomalous trend in frequency and linewidth of this low frequency phonon to the electron-phonon coupling. Furthermore, our work also highlights the temperature induced tuning of resonance condition via understanding the intensity of phonon modes as a function of temperature.

Quantum spin liquid (QSL), a state characterized by exotic low energy fractionalized excitations and statistics is still elusive experimentally and may be gauged via indirect experimental signatures. Remnant of QSL phase may reflect in the spin dynamics as well as quanta of lattice vibrations, i.e., phonons, via the strong coupling of phonons with the underlying fractionalized excitations i.e., Majorana fermions. Inelastic light scattering (Raman) studies on V1-xPS3 single crystals evidences the spin fractionalization into Majorana fermions deep into the paramagnetic phase reflected in the emergence of a low frequency quasielastic response along with a broad magnetic continuum marked by a crossover temperature T* ~ 200 K from a pure paramagnetic state to fractionalized spins regime qualitatively gauged via dynamic Raman susceptibility. We further evidenced anomalies in the phonons self-energy parameters in particular phonon line broadening and line asymmetry evolution at this crossover temperature, attributed to the decaying of phonons into itinerant Majorana fermions. This anomalous scattering response is thus indicative of fluctuating fractionalized spins suggesting a phase proximate to the quantum spin liquid state in this quasi two-dimensional (2D) magnetic system.

Excitonic quasi-particles, excitons/trions/bi-excitons, and their coupling with phonons and charge carriers play a crucial role in controlling the optical properties of atomically thin semiconducting 2D materials. In this work, we unravelled the dynamics of excitons/trions and their coupling with phonons and charge carriers in a few layers vertically and horizontally aligned MoS2. We observed trion signature up to the highest recorded temperature (330 K) in both systems and have shown that the dynamics of excitons/trions and their coupling with phonons and electrons are more affected in vertically aligned MoS2. A homogeneous linewidth broadening is observed with an increase in temperature. The linewidth broadening is attributed mainly to acoustic phonons in a low-temperature regime (<100 K). In contrast, acoustic and longitudinal optical phonons contributions to the linewidth broadening are observed at high temperature. We also observed the significant effects of interlayer coupling in both systems via understanding the temperature-dependent valence band splitting and trion binding energy. A decrease of 22 and 12% in valence band splitting with temperature rise is observed for the vertically and horizontally aligned MoS2, respectively, suggesting that the valence band splitting is affected more in the case of vertically than horizontally aligned. Furthermore, we also notice a significant thermal quenching in the intensity of the trion band than that of exciton bands, attributed to the small binding energy of the trion.

Probing phonons, quasi-particle excitations and their coupling has enriched our understanding of these 2D materials and proved to be crucial for developing their potential applications. Here, we report comprehensive temperature, 4-330 K, and polarization-dependent Raman measurements on mono and bilayer MoSe2. Phonon's modes up to fourth-order are observed including forbidden Raman and IR modes, understood considering Frohlich mechanism of exciton-phonon coupling. Most notably, anomalous variations in the phonon linewidths with temperature pointed at the significant role of electron-phonon coupling in these systems, especially for the out-of-plane (A1g) and shear mode (E22g), which is found to be more prominent in the narrow-gaped bilayer than the large gapped monolayer. Via polarization-dependent measurements, we deciphered the ambiguity in symmetry assignments, especially to the peaks around ~ 170 cm-1 and ~ 350 cm-1. Temperature-dependent thermal expansion coefficient, an important parameter for the device performance, is carefully extracted for both mono and bilayer by monitoring the temperature-dependence of the real-part of the phonon self-energy parameter. Our temperature-dependent in-depth Raman studies provide a pave for uncovering the deeper role of phonons in these 2D layered materials from a fundamental as well as application point of view.

We present a comprehensive temperature dependent Raman measurements for horizontally aligned CVD grown layered MoS2 in a temperature range of 4 to 330 K under resonance condition. Our analysis of temperature dependent phonon frequency shift and linewidth suggest a finite role of three and four phonon anharmonic effect. We observed Davydov splitting of the out-of-plane (A1g ) and in-plane (E12g ) modes, attributed to the weak interlayer interaction, and reflected in the appearance of additional modes with decreasing temperature for both 3 layers and few layers system. We also observed that the number of Davydov splitting components are more in few layers as compared to 3L MoS2, suggesting it increases with increasing number of layers. Temperature evaluation of the Raman spectra shows that the Davydov splitting, especially for A1g mode, is very strong and well resolved at low temperature. We note that A1g mode shows splitting at low temperature, while E12g mode is splitted even at room temperature, and that suggests to prominent role of A1g mode to the interlayer interaction. Further, the temperature dependence tuning of resonance effect is observed, via almost sixty fold increase in the intensity of the phonon modes at low temperature.

Hitherto, the discrete identification of quantum spin liquid phase, holy grail of condensed matter physics, remains a challenging task experimentally. However, the precursor of quantum spin liquid state may reflect in the spin dynamics even in the paramagnetic phase over a wide temperature range as conjectured theoretically. Here we report comprehensive inelastic light (Raman) scattering measurements on the Ir based double perovskite, Gd2ZnIrO6, as a function of different incident photon energies and polarization in a broad temperature range. Our results evidenced the spin fractionalization within the paramagnetic phase reflected in the emergence of a polarization independent quasi-elastic peak at low energies with lowering temperature. Also, the fluctuating scattering amplitude measured via dynamic Raman susceptibility increases with lowering temperature and decreases mildly upon entering into long-range magnetic ordering phase, below 23 K, suggesting the magnetic origin of these fluctuations. This anomalous scattering response is thus indicative of fluctuating fractional spin evincing the quantum spin liquid phase in a three-dimensional double perovskite system., Comment: 3 figures

Transition metal dichalcogenide, especially MoS2 has attracted lot of attention recently owing to its tunable visible range band gap and anisotropic electronic and transport properties. Here, we report a comprehensive inelastic light scattering measurements on CVD grown (horizontally and vertically aligned flakes) as well as single crystal flakes of MoS2, probing the anisotropic optical response via studying the polarization dependence intensity of the Raman active phonon modes as a function of different incident photon energy and flake thickness. Our polarization dependent Raman studies intriguingly revealed strong anisotropic behavior reflected in the anomalous renormalization of the modes intensity as a function of flake thickness, phonons and photon energy. Our observations reflects the strong anisotropic light-matter interaction in this high crystalline symmetric layered MoS2 system especially for the in-plane vibrations, which is crucial for understanding as well application of these materials for future application such as optoelectronic applications.

We report a comprehensive temperature dependent Raman measurements on three different phases of monolayer WS2 from 4K to 330K in a wide spectral range. Our studies revels the anomalous nature of the first as well as the higher order combination modes reflected in the disappearance of the few modes and anomalous temperature evaluation of the phonon self-energy parameters attributed to the detuning of resonance condition and development of strain due to thermal expansion mismatch with the underlying substrate. Our detailed temperature dependence studies also decipher the ambiguity about assignment of the two modes in literature near ~ 297 cm-1 and 325 cm-1. Mode near 297 cm-1 is assigned as first order Raman mode, which is forbidden in the backscattering geometry and 325 cm-1 is assigned to the combination of and mode. We also estimated thermal expansion coefficient by systematically disentangling the substrate effect in the temperature range of 4K to 330K and probed its temperature dependence in 1H, 1T and 1T' phases., Comment: 24 pages, 6 Figures

Conventional Paramagnetism - a state with finite magnetic moment per ion sans long range magnetic ordering, but with lowering temperature the moment on each ion picks up a particular direction, breaking rotational symmetry, and results into long range magnetic ordering. However, in systems with competing multiple degrees of freedom this conventional notion may easily breaks and results into short range correlation much above the global magnetic transition temperature. La2CuIrO6 with complex interplay of spins (s =1/2) on Cu site and pseudo-spin (j =1/2) on Ir site owing to strong spin-orbit coupling provides fertile ground to observe such correlated phenomena. By a comprehensive temperature dependent Raman study, we have shown the presence of such a correlated paramagnetic state in La2CuIrO6 much above the long range magnetic ordering temperature (TN ). Our observation of strong interactions of phonons, associated with Cu/Ir octahedra, with underlying magnetic degrees of freedom mirrored in the observed Fano asymmetry, which remarkably persists as high as ~ 3.5TN clearly signals the existence of correlated paramagnetism hence broken rotational symmetry. Our detailed analysis also reveals anomalous changes in the self-energy parameters of the phonon modes, i.e. mode frequencies and linewidth, below TN, providing a useful gauge for monitoring the strong coupling between phonons and magnetic degrees of freedom., Comment: 22 pages, 6 figures

Structural, vibrational and dielectric properties of (Pb1-xBix)(Ti1-xMnx)O3 (PBTM) (0 x 0.50) polycrystalline ceramics have been examined as a function of temperature. Synchrotron-based powder x-ray diffraction was employed to confirm phase purity and crystal structure of samples. Tetragonality (c/a ratio) of the PBTM system exhibit an increase 1.065, 1.066 for x = 0.06 and 0.09 compositions respectively, compare to 1.064 for x = 0 sample. Curie point was found ~763 K and 773 K for x = 0.06 and 0.09 samples respectively. Though, tetragonality start to decreasing from samples with x 0.18, Curie point of the samples started decreasing for x 0.12. Temperature-dependent x-ray diffraction reveals the structural change from tetragonal to cubic structure. Unit cell volume was found to decrease with increasing temperature; indicate these materials are negative thermal expansion type until phase transition temperature, with negative thermal coefficients are -1.571*10-5 /K, -2.44*10-5 /K, and -5.025*10-6 /K for x = 0, 0.06, and 0.09 samples respectively. Raman spectra showed softening of the transverse optical phonon modes and increase in the full width at half maxima with the increase in composition. Field-emission scanning electron microscope equipped with energy dispersive x-ray spectrometer (EDS) confirmed compositional homogeneity and dense type microstructure., Comment: 26 pages, 12 figures