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P. Lemmens

Publications and source records attributed to P. Lemmens.

At least 19 recordsLinked to original sources

Optical phonons as a testing ground for spin group symmetries

Lattice vibrations are highly sensitive to crystal symmetries and their changes across phase transitions. The latter can modify irreducible (co)representations and corresponding infrared and Raman selection rules of phonons. This concept is established for relativistic magnetic point groups, simultaneously transforming spatial and spin coordinates. However, in altermagnets described by non-relativistic spin groups with disjunct symmetry operations for both vector spaces, the phonon selection rules have remained unexplored. Here, we present a detailed study of the infrared- and Raman-active modes in the collinear antiferromagnet and altermagnet candidate Co$_2$Mo$_3$O$_8$. Comparing to ab initio calculations accurately capturing the eigenfrequencies, we identify all expected phonon modes at room temperature and deduce their selection rules using both symmetry approaches. Importantly, we observe the change of selection rules upon antiferromagnetic ordering, agreeing with the relativistic symmetry approach, while the spin group formalism predicts no changes. Therefore, optical phonons can reveal the appropriate symmetry treatment.

cond-mat.mtrl-sci

Phase separation and phase transitions in undoped and Rh3+ doped iron pnictide CaFe2As2: a Raman scattering study

Iron-pnictides Ca(Fe1-xRhx)2As2 (x = 0, 0.035, and 0.19) were studied across the tetragonal-orthorhombic and uncollapsed to collapsed tetragonal phase transitions using Raman spectroscopy. The effect of the phase separation was observed in the high-temperature phase for the first time. Two phases with the low-spin and high-spin states of the Fe2+ ions coexist in the undoped (x = 0) and doped (x = 0.035) samples at ambient conditions. These two phases are present on a larger length scale and they are not limited to the local distortions. Both phases in the undoped sample successfully undergo tetra-to-ortho phase transitions approximately at the same temperature T0 = 160 K. In doped samples, a cascade of phase transitions is observed at temperatures T* = 100 K and Tc = 72 K with cooling for the first time. A complex type of the re-entrant magnetic structure is realized in the x = 0.035 sample at temperatures below Tc, which is distinct from the usual orthorhombic twofold one. The overdoped sample (x = 0.19) also shows phase separation at temperatures 7 - 295 K in Raman spectra similar to these of the remnant phase.

cond-mat.supr-con

Kitaev Spin Liquid Candidate OsxCl3 Comprised of Honeycomb Nano-Domains

An osmium chloride with the chemical formula of OsxCl3 (x = 0.81) was synthesized and its crystal structure and thermodynamic properties were investigated. OsxCl3 crystallizes in a layered CdCl2-type structure with the triangular lattice partially occupied by Os ions on average. However, on microscopic length scales, the triangular lattice is composed of nano-domains with a honeycomb arrangement of Os ions, as observed by electron microscopy and Raman scattering experiments. Magnetization and heat capacity measurements revealed an absence of magnetic long-range order down to 0.08 K, while a broad peak in heat capacity at 0.15 K may indicate a short-range order in the local honeycomb lattice. OsxCl3 may exhibit certain aspects of the Kitaev spin liquid that are expected for a perfect honeycomb lattice of osmium trichloride.

cond-mat.str-el

Flat-band spin dynamics and phonon anomalies of the saw-tooth spin-chain system Fe$_2$O(SeO$_3$)$_2$

Fe$^{3+}$ $S = 5/2$ ions form saw-tooth like chains along the $a$ axis of the oxo-selenite Fe$_2$O(SeO$_3$)$_2$ and an onset of long-range magnetic order is observed for temperatures below $T_C = 105$ K. This order leads to distinct fingerprints in phonon mode linewidths and energies as resolved by Raman scattering. In addition, new excitations with small linewidths emerge below $T = 150$ K, and are assigned to two-magnon scattering processes with the participation of flat-band and high energy magnon branches. From this a set of exchange coupling constants is estimated. The specific ratio of the saw-tooth spine-spine and spine-vertex interactions may explain the instability of the dimer quantum ground state against an incommensurate 3D magnetic order.

cond-mat.str-el

Soft tilt and rotational modes in the hybrid improper ferroelectric Ca$_{3}$Mn$_{2}$O$_{7}$

Raman spectroscopy is employed to probe directly the soft rotation and tilting modes, which are two primary order parameters predicted in the hybrid improper ferroelectric material Ca$_3$Mn$_2$O$_7$. We observe a giant softening of the 107-cm$^{-1}$ octahedron tilting mode by 26~cm$^{-1}$, on heating through the structural transition from a ferroelectric to paraelectric orthorhombic phase. This is contrasted by a small softening of the 150-cm$^{-1}$ rotational mode by 6~cm$^{-1}$. In the intermediate phase, the competing soft modes with different symmetries coexist, bringing about many-faceted anomalies in spin excitations and lattice vibrations. Our work demonstrates that the soft rotation and tilt patterns, relying on a phase-transition path, are a key factor in determining ferroelectric, magnetic, and lattice properties of Ca$_3$Mn$_2$O$_7$.

cond-mat.str-el

Quantum criticality in the coupled two-leg spin ladder Ba2CuTeO6

We report on zero-field muon spin rotation, electron spin resonance and polarized Raman scattering measurements of the coupled quantum spin ladder Ba2CuTeO6. Zero-field muon spin rotation and electron spin resonance probes disclose a successive crossover from a paramagnetic through a spin-liquid-like into a magnetically ordered state with decreasing temperature. More significantly, the two-magnon Raman response obeys a T-linear scaling relation in its peak energy, linewidth and intensity. This critical scaling behavior presents an experimental signature of proximity to a quantum critical point from an ordered side in Ba2CuTeO6.

cond-mat.str-el

Relation between Kitaev magnetism and structure in $α$-RuCl$_3$

Raman scattering has been employed to investigate lattice and magnetic excitations of the honeycomb Kitaev material $α$-RuCl$_3$ and its Heisenberg counterpart CrCl$_3$. Our phonon Raman spectra give evidence for a first-order structural transition from a monoclinic to a rhombohedral structure for both compounds. Significantly, only $α$-RuCl$_3$ features a large thermal hysteresis, consistent with the formation of a wide phase of coexistence. In the related temperature interval of $70-170$ K, we observe a hysteretic behavior of magnetic excitations as well. The stronger magnetic response in the rhombohedral compared to the monoclinic phase evidences a coupling between the crystallographic structure and low-energy magnetic response. Our results demonstrate that the Kitaev magnetism concomitant with fractionalized excitations is susceptible to small variations of bonding geometry.

cond-mat.str-el

Optical phonon dynamics and electronic fluctuations in the Dirac semimetal Cd3As2

Raman scattering in the three-dimensional Dirac semimetal Cd3As2 shows an intricate interplay of electronic and phonon degrees of freedom. We observe resonant phonon scattering due to interband transitions, an anomalous anharmonicity of phonon frequency and intensity, as well as quasielastic (E~0) electronic scattering. The latter two effects are governed by a characteristic temperature scale T* ~ 100 K that is related to mutual fluctuations of lattice and electronic degrees of freedom. A refined analysis shows that this characteristic temperature corresponds to the energy of optical phonons which couple to interband transitions in the Dirac states of Cd3As2. As electron-phonon coupling in a topological semimetal is primarily related to phonons with finite momenta, the back action on the optical phonons in only observed as anharmonicities via multi-phonon processes involving a broad range of momenta. The resulting energy density fluctuations of the coupled system have previously only been observed in low dimensional or frustrated spin systems with suppressed long range ordering.

cond-mat.mtrl-sci

Raman spectroscopic signature of fractionalized excitations in the harmonic-honeycomb iridates $β$- and $γ$-Li$_2$IrO$_3$

The fractionalization of elementary excitations in quantum spin systems is a central theme in current condensed matter physics. The Kitaev honeycomb spin model provides a prominent example of exotic fractionalized quasiparticles, composed of itinerant Majorana fermions and gapped gauge fluxes. However, identification of the Majorana fermions in a three-dimensional honeycomb lattice remains elusive. Here we report spectroscopic signatures of fractional excitations in the harmonic-honeycomb iridates $β$- and $γ$-Li$_2$IrO$_3$. Using polarization resolved Raman spectroscopy, we find that the dynamical Raman response of $β$- and $γ$-Li$_2$IrO$_3$ features a broad scattering continuum with distinct polarization and composition dependence. The temperature dependence of the Raman spectral weight is dominated by the thermal damping of fermionic excitations. These results suggest the emergence of Majorana fermions from spin fractionalization in a three-dimensional Kitaev-Heisenberg system.

cond-mat.str-el

Phase separation in iron chalcogenide superconductor Rb0.8+xFe1.6+ySe2 as seen by Raman light scattering and band structure calculations

We report Raman light scattering in the phase separated superconducting single crystal Rb0.77Fe1.61Se2 with Tc = 32 K. The spectra have been measured in a wide temperature range 3K -500K. The observed phonon lines from the majority vacancy ordered Rb2Fe4Se5 (245) antiferromagnetic phase with TN= 525 K demonstrate modest anomalies in frequency, intensity and halfwidth at the superconductive phase transition. We identify phonon lines from the minority compressed RbδFe2Se2 (122) conductive phase. The superconducting gap with dx2-y2 symmetry is also detected in our spectra. In the range 0-600 cm-1 we observed the low intensive but highly polarized B1g-type background which becomes well structured under cooling. The possible magnetic or multiorbital origin of this background has been discussed. We argue that phase separation in M0.8+xFe1.6+ySe2 has pure magnetic origin. It occurs below Neel temperature when iron magnetic moment achieves some critical magnitude. We state that there is a spacer between the majority 245 and minority 122 phases. Using ab-initio spin polarized band structure calculations we demonstrate that compressed vacancy ordered Rb2Fe4Se5 phase can be conductive and therefore may serve as a protective interface spacer between the pure metallic RbδFe2Se2 phase and the insulating Rb2Fe4Se5 phase providing the percolative Josephson-junction like superconductivity in the whole sample of Rb0.8+xFe1.6+ySe2 Our lattice dynamics calculations show significant difference in the phonon spectra of the conductive and insulating Rb2Fe4.Se5 phases.

cond-mat.supr-con

Longitudinal magnon, inversion breaking and magnetic instabilities in the pseudo-Kagome francisites Cu3Bi(SeO3)2O2X with X=Br, Cl

We performed Raman studies and a dielectric characterization of the pseudo-kagome Cu3Bi(SeO3)2O2X (X = Cl, Br). These compounds share competing nearest-neighbour ferromagnetic exchange and frustrating next-nearest-neighbour antiferromagnetic exchange as well as highly noncollinear magnetic ground state. However, at low temperature they differ with respect to the existence of inversion symmetry. For both compounds there exists a pronounced interplay of polar phonon modes with quantum magnetic fluctuations. A novel Raman mode appears for temperatures below the Neel temperature with a Fano lineshape and an enormous intensity that exceeds most of the phonon lines. We discuss a possible contribution of longitudinal magnons to this signal. In contrast, one magnon scattering based on linear transvers magnons is excluded based on a symmetry analysis of spin wave representations and Raman tensor calculations. There exists evidence that in these pseudo-kagome compounds magnetic quantum fluctuations carry an electric dipole moment. Our data as well as a comparison with previous far-infrared spectra allow us to conclude that Cu3Bi(SeO3)2O2Cl changes its symmetry most likely from Pmmn to P21mn with a second order structural phase transition at T*=120 K and becomes multiferroic. Cu3Bi(SeO3)2O2Br represents an interesting counter part as it does not show this instability and stays inversion symmetric down to lowest temperatures, investigated.

cond-mat.str-el

Enhanced quasiparticle dynamics of quantum well states: the giant Rashba system BiTeI and topological insulators

In the giant Rashba semiconductor BiTeI electronic surface scattering with Lorentzian linewidth is observed that shows a strong dependence on surface termination and surface potential shifts. A comparison with the topological insulator Bi2Se3 evidences that surface confined quantum well states are the origin of these processes. We notice an enhanced quasiparticle dynamics of these states with scattering rates that are comparable to polaronic systems in the collision dominated regime. The Eg symmetry of the Lorentzian scattering contribution is different from the chiral (RL) symmetry of the corresponding signal in the topological insulator although both systems have spin-split surface states.

cond-mat.str-el

Specific features of electron spin resonance in quasi-1D magnet β-TeVO4

The angular and temperature dependences of single crystal ESR spectra at X-band frequency of quasi 1D spin 1/2 antiferromagnetic zigzag chain system β-TeVO4 are reported. Two resonance components in the ESR spectrum have been detected: a weak narrow resonance on the top of the extremely broad signal. The narrow line might be due to an impurity, the characteristics of the broad absorption do not correlate with a picture of the typical behavior for the V4+ ions (S = 1/2) with a square pyramidal environment. It was found that at low temperatures the divergence of the spin susceptibility and linewidth of the observed excitations can be due to a realization of three dimensional magnetic ordering.

cond-mat.str-el

Enhanced low energy fluctuations and increasing out-of-plane coherence in vacancy ordered NaxCoO2

We report Raman scattering experiments on the strongly correlated electron system NaxCoO2 with x= 0.71 and ordered Na vacancies. In this doping regime, NaxCoO2 exhibits a large and unusual thermopower and becomes superconducting upon hydration. Our Raman scattering data reveal pronounced low energy fluctuations that diverge in intensity at low temperatures. Related to these fluctuations is a drastic decrease of an electronic scattering rate from 50 to 3 cm-1. This observation is quite different from the behavior of Na disordered samples that have a larger and temperature independent scattering rate. Simultaneously with the evolution of the scattering rate, phonon anomalies point to an increasing out-of-plane coherence of the lattice with decreasing temperature. These observations may indicate the condensation of spin polarons into an unusual, highly dynamic ground state.

cond-mat.str-el

Evidence for Dimer Crystal Melting in the Frustrated Spin-Ladder BiCu2PO6

In the spin ladder compound BiCu$_2$PO$_6$ there exists a decisive dynamics of spin excitations that we classify and characterize using inelastic light scattering. We observe low-energy singlets and a broad triplon continuum extending from 36 cm$^{-1}$ to 700 cm$^{-1}$ in ($aa$), ($bb$), and ($cc$) light scattering polarizations. Though isolated spin ladder physics can roughly account for the observed excitations at high energies, frustration and interladder interactions need to be considered to fully describe the spectral distribution and scattering selection rules at low and intermediate energies. More significantly, an interladder singlet bound mode at 24 cm$^{-1}$, lying below the continuum, shows its largest scattering intensity in interladder ($ab$) polarization. In contrast, two intraladder bound states at 62 cm$^{-1}$ and 108 cm$^{-1}$ with energies comparable to the continuum are observed with light polarization along the leg ($bb$) and the rung ($cc$). We attribute the rich spectrum of singlet bound modes to a melting of a dimer crystal. Our study provides evidence for a Z$_2$ quantum phase transition from a dimer to a resonating valence bond state driven by singlet fluctuations.

cond-mat.str-el

Coupling of spin and lattice modes in the S=1/2 two-dimensional antiferromagnet K$_{2}$V$_{3}$O$_{8}$ with magneto-dielectric couplings

Lattice dynamics and magnetic excitations are investigated to elucidate the origin of magneto-dielectric effects in the S=1/2 two-dimensional quantum spin compound K$_2$V$_3$O$_8$. We find evidence for lattice instabilities at 110 K and 60 K as optical phonon anomalies and a soft mode at 26 cm$^{-1}$ in A$_1$ symmetry. Two-magnon excitations in B$_1$ symmetry show an unconventional double-peak structure and temperature dependence. This suggests the existence of a split mode near the zone boundary caused by a mixing of spin and lattice modes.

cond-mat.str-el

Long wavelength helimagnetic order and skyrmion lattice phase in Cu2OSeO3

We report a long-wavelength helimagnetic superstructure in bulk samples of the ferrimagnetic insulator Cu2OSeO3. The magnetic phase diagram associated with the helimagnetic modulation inferred from small angle neutron scattering and magnetisation measurements includes a skyrmion lattice phase and is strongly reminiscent of MnSi, FeGe and Fe1-xCoxSi, i.e., binary isostructural siblings of Cu2OSeO3 that order helimagnetically. The temperature dependence of the specific heat of Cu2OSeO3 is characteristic of nearly critical spin fluctuations at the helimagnetic transition. This provides putative evidence for effective spin currents as the origin of enhancements of the magneto-dielectric response instead of atomic displacements considered so far.

cond-mat.str-el

Dynamical lattice instability versus spin liquid state in a frustrated spin chain system

The low-dimensional s=1/2 compound (NO)[Cu(NO3)3] has recently been suggested to follow the Nersesyan-Tsvelik model of coupled spin chains. Such a system shows unbound spinon excitations and a resonating valence bond ground state due spin frustration. Our Raman scattering study demonstrates phonon anomalies as well as the suppression of a broad magnetic scattering continuum for temperatures below a characteristic temperature, T<T*=100K. We interpret these effects as evidence for a dynamical interplay of spin and lattice degrees of freedom that might lead to a further transition into a dimerized or structurally distorted phase at lower temperatures.

cond-mat.str-el