Polarization-resolved Raman spectroscopy was performed and analyzed from large, high quality, mono-domain single crystal of α-RuCl3, a proximate Kitaev quantum spin liquid. Spectra were collected with laser polarizations parallel and perpendicular to the honeycomb plane. Pairs of nearly degenerate phonons were discovered and show either a 4-fold or 2-fold polarization angle dependence in their Raman intensity, thereby providing evidence to definitively assign the bulk crystal point group as C2h. The low frequency continuum that is often attributed to scattering from pairs of Majorana fermions was also examined and found to disappear when the laser excitation and scattered photon polarizations were perpendicular to the honeycomb plane. This disappearance, along with the behavior of the phonon spectrum in the same polarization configuration, strongly suggests that the scattering continuum is 2-dimensional. We argue that this scattering continuum originates from the Kitaev magnetic interactions that survives up to room temperature, a scale larger than the bare Kitaev exchange energy of approximately 50 K.
Ultrafast characterization and control of many-body interactions and elementary excitations are critical to understanding and manipulating emergent phenomena in strongly correlated systems. In particular, spin interaction plays an important role in unconventional superconductivity, but efficient tools for probing spin dynamics especially out of equilibrium, are still lacking. To address this question, we develop a theory for nonresonant time-resolved Raman scattering, which can be a generic and powerful tool for nonequilibrium studies. We also use exact diagonalization to simulate the pump-pro…
The phonon dynamics of LiV2O5 single crystals is studied using infrared and Raman spectroscopy techniques. The infrared-active phonon frequencies and dielectric constants are obtained by oscillator fitting procedure of the reflectivity data measured at room temperature. The Raman scattering spectra are measured at room temperature and at T=10 K in all nonequivalent polarized configurations. The assignment of the phonons is done by comparing the infrared and Raman spectra of LiV2O5 and NaV2O5. The factor-group-analysis of the LiV2O5 crystal symmetry and of its constituent layers is performed to…
Measurement and control of magnetic order and correlations in real time is a rapidly developing scientific area relevant for magnetic memory and spintronics [1,15]. In these experiments an ultra-short laser pulse (pump) is first absorbed by excitations carrying electric dipole moment. These then give their energy to the magnetic subsystem monitored by a time-resolved probe. A lot of progress has been made in investigations of ferromagnets but antiferromagnets are more challenging. Here we introduce time-resolved two-magnon Raman scattering as a novel real time probe of magnetic correlations es…
We investigate a momentum-resolved Raman spectroscopy technique which is able to probe the one-body spectral function and the quasi-particle states of a gas of strongly interacting ultracold atoms. This technique is inspired by Angle-Resolved Photo-Emission Spectroscopy, a powerful experimental probe of electronic states in solid-state systems. Quantitative examples of experimentally accessible spectra are given for the most significant regimes along the BEC-BCS crossover. When the theory is specialized to RF spectroscopy, agreement is found with recent experimental data. The main advantages o…
We present a polarization-resolved and temperature-dependent Raman scattering study of AFe2As2 (A = Ca, Eu). In the spin-density-wave (SDW) phase, spectral weight redistribution is observed in the fully symmetric and non-symmetric scattering channels at different energies. An anisotropic Raman response is observed in the fully symmetric channel in spontaneously detwinned CaFe2As2 samples. We calculate the orbital-resolved electronic structures using a combination of density functional theory and dynamical mean field theory (DFT+DMFT). We identify the electronic transitions corresponding to the…
We study the dynamics of the superconducting order parameter in the high-$T_c$ cuprate Bi$_2$Sr$_2$CaCu$_2$O$_{8-δ}$ by employing a novel time-resolved pump-probe Raman experiment. We find two different coupling mechanisms that contribute equally to the pair breaking peak. One coupling sets in very fast at 2ps and relaxes slow, while the other one is delayed and sets in roughly at 5ps and relaxes fast. A model that couples holes through phonons is able to reproduce one part of the condensate dynamics, thus, we argue that hole-spin interactions are of importance as well.
We report on a study of the inelastic scattering properties of (001) and (111) Ho$_2$Ti$_2$O$_7$ single crystals at room temperature. Structural and compositional analysis along with absorption measurement confirms single crystalline phase of all samples. Room temperature polarized Raman measurements were performed on crystals in non-resonant and two different resonant conditions by using six different laser excitation lines. Lorentzian model fitting analysis is performed on all measured spectra in order to identify the difference in the Raman scattering cross-section in resonant and non-reson…
We explain quantitatively why resonant Raman scattering spectroscopy, an extensively used experimental tool in studying elementary electronic excitations in doped low dimensional semiconductor nanostructures, always produces an observable peak at the so-called "single particle" excitation although the standard theory predicts that there should be no such single particle peak in the Raman spectra. We have thus resolved an experimental puzzle which dates back more than twenty-five years.
We performed an optical spectroscopy study of electronic and magnetic excitations for a rare-earth system with a single electron quasi-localized in the f-shell on an ion at high-symmetry crystallographic site in application to CeB$_{6}$ heavy-fermion metal. We carried out group-theoretical classification of the electronic crystal field (CF) transitions and assessed their coupling to light cross-sections for polarization resolved Raman scattering processes. We discuss applicability of symmetrized Raman susceptibility to studies of exotic charge and spin high multiplet ordering phases in f-elect…
Monoclinic semi-metallic Mo$_8$O$_{23}$ belongs to a multifunctional series of compounds showing multiple ordering phenomena that have not achieved much attention till now. Previous X-rays studies of this compound have revealed an incommensurate ordering transition at $T_{\mathrm{IC}}\sim350$ K, followed by a structural transition to commensurate order at $T_{\mathrm{IC-C}}=285$ K. In addition, an enigmatic resistance maximum is observed at $T_{\mathrm{el}}\sim150$ K, whose origin has so far proved elusive. Aiming to disentangle these multiple orders we use the polarized transient optical spec…
We report for the first time, that Fe3Se4 is a room temperature, type-II multiferroic with magnetoelectric coupling. We observed the coexistence of coupled ferrimagnetic and ferroelectric ordering in Fe3Se4nanorods well above room temperature, which is a hard magnet with large magnetocrystalline anisotropy. For the first time, we observed spontaneous, reversible ferroelectric polarization in Fe3Se4 nanorods below the magnetic Curie temperature. The coupling is manifested by an anomaly in the dielectric constant and Raman shift at Tc. We do not completely understand the origin of the ferroelect…
Both electronic Raman scattering (ERS) and angle-resolved photoemission spectra (ARPES) revealed two energy scales for the gap in different momentum spaces in the cuprates. However, the interpretations were different, and the gap values were also different in two experiments. In order to clarify the origin of these discrepancies, we directly compared ERS and ARPES by calculating ERS from the experimental data of ARPES through the Kubo formula. The calculated ERS spectra were in good agreement with the experimental results except for the B$_{1g}$ peak energies. The doping-dependent B$_{2g}$ pea…
Contrasting anisotropic electron-phonon-spin coupling in Fe$_{3}$GeTe$_{2}$ and Fe$_{5}$GeTe$_{2}$: A helicity-resolved Raman study
Indian Institute of Technology Kharagpur（印度理工学院卡拉格普尔分校）；Jawaharlal Nehru University（贾瓦哈拉尔·尼赫鲁大学）；Institute of Nuclear Physics, Polish Academy of Sciences（波兰科学院核物理研究所）；Sungkyunkwan University（成均馆大学）
We measured the optical signature of the charge density waves (CDWs) in the multiband conductor TTF[Ni(dmit)2]2 by electronic Raman scattering. At low energies, a hump develops below 60 K. This hump is associated to the amplitude mode of the CDW with an energy around 9 meV. Raman symmetry-resolved measurements show that the CDW amplitude mode is anisotropic and that the CDW can be associated to the band nesting of Ni(dmit)2 chains.
The Channel-Spark method was used for deposition of highly oriented ferromagnetic La0.7Sr0.3MnO3 films on NdGaO3 substrates. It was found that additional oxygen decreases the film quality suppressing the Curie temperature and metal-insulator transition below the room temperature. To achieve the best quality of the films the samples were either annealed in high vacuum at deposition temperature or even deposited in argon atmosphere with no oxygen annealing. For such films the resistive measurements showed a metallic behaviour in the interval 10-300 K in accordance with the high Curie point (Tc 3…
We report a Raman scattering study of nematic degrees of freedom in the iron-based superconductor parent compound BaFe$_2$As$_2$ under tunable uniaxial strain. We demonstrate that the polarization resolved arsenic (As) phonon intensity can be used to monitor the nematic order parameter as a function of both temperature and strain. At low temperature in the nematic ordered phase we use it to track the continuous and reversible orientation of nematic domains under variable strain. At higher temperature, the evolution of the As phonon intensity under strain reflects an enhanced nematic susceptibi…
We report on the first optical characterization of both cubic and hexagonal SrMnO$_3$. Room-temperature Raman spectra collected by means of a micro-Raman spectrometer are shown. The spectrum of the cubic compound is characterized by weak and broad bands in agreement with group-theory which predicts no Raman-active phonons for this compound. On the other hand, the spectrum of the hexagonal compound shows six narrow peaks ascribed to one-phonon processes. A complete polarization analysis of the spectra collected from a single crystallite allows us to completely assign the symmetries of the six o…
Raman scattering experiments on Na_{x}CoO_2 yH_2O single crystals show a broad electronic continuum with a pronounced peak around 100 cm-1 and a cutoff at approximately 560 cm-1over a wide range of doping levels. The electronic Raman spectra in superconducting and non-superconducting samples are similar at room temperature, but evolve in markedly different ways with decreasing temperature. For superconducting samples, the low-energy spectral weight is depleted upon cooling below T* sim 150K, indicating a opening of a pseudogap that is not present in non-superconducting materials. Weak addition…
We reported two-magnon Raman scattering from La_{1.9}Sr_{0.1}CuO_4, which has a suppressed Tc=12 K, as the temperature is lowered below 37 K and an ordered spin phase is formed. The two-magnon Raman intensity increases with decreasing temperature. The magnetic scattering in La_{1.9}Sr_{0.1}CuO_4 is totally different from that reported in the parent compound La_2CuO_4. We analyze the line shape of the two-magnon scattering within the traditional Loudon-Fleury theory and find the superexchange constant J=1052 cm^{-1}. The calculation of the frequency moment suggests that the quantum fluctuations…
Graphene layers placed on SrTiO3 single-crystal substrates were investigated using temperature-dependent confocal Raman spectroscopy. This approach successfully resolved distinct Raman modes of graphene that are often untraceable in conventional measurements due to the strong Raman scattering background of SrTiO3. Information on defects and strain states was obtained for a few graphene/SrTiO3 samples that were synthesized by different techniques. This confocal Raman spectroscopic approach can shed light on the investigation of not only this graphene/SrTiO3 system but also various two-dimension…
