arXiv subjects

S. Raymond

Publications and source records attributed to S. Raymond.

At least 37 records · Page 2Linked to original sources

arXiv2020

Direct evidence of weakly dispersed and strongly anharmonic optical phonons in hybrid perovskites

Hybrid organolead perovskites (HOP) have started to establish themselves in the field of photovoltaics, mainly due to their great optoelectronic properties and steadily improving solar cell efficiency. Study of the lattice dynamics is key in understanding the electron-phonon interactions at play, responsible for such properties. Here, we investigate, via neutron and Raman spectroscopies, the optical phonon spectrum of four different HOP single crystals: MAPbBr$_3$, FAPbBr$_3$, MAPbI$_3$, and $α$-FAPbI$_3$. Low temperature spectra reveal weakly dispersive optical phonons, at energies as low as 2-5~meV, which seem to be the origin of the limit of the charge carriers mobilities in these materials. The temperature dependence of our neutron spectra shows as well a significant anharmonic behaviour, resulting in optical phonon overdamping at temperatures as low as 80~K, questionning the validity of the quasi-particle picture for the low energy optical modes at room temperature where the solar cells operate.

cond-mat.mtrl-sci↗

arXiv2019

Presaturation phase with no dipolar order in a quantum ferro-antiferromagnet

Magnetization, magnetocaloric, calorimetric, neutron and X-ray diffraction and inelastic neutron scattering measurements are performed on single crystals of BaCdVO(PO$_4$)$_2$. The low-temperature crystal structure is found to be of a lower symmetry than previously assumed. The result is a more complicated model spin Hamiltonian, which we infer from measurements of the spin wave dispersion spectrum. The main finding is a novel spin state which emerges in high magnetic fields after antiferromagnetic order is terminated at $H_{c1}\simeq 4.0$ T. It is a distinct thermodynamic phase with a well-defined phase boundary at $H_{c2}\simeq 6.5$ T and is clearly separate from the fully saturated phase. Yet, it shows no conventional (dipolar) magnetic long range order. We argue that it is fully consistent with the expectations for a quantum bond-nematic state.

cond-mat.str-el↗

arXiv2019

Evolution of Magnetic Order from the Localized to the Itinerant Limit

Quantum materials that feature magnetic long-range order often reveal complex phase diagrams when localized electrons become mobile. In many materials magnetism is rapidly suppressed as electronic charges dissolve into the conduction band. In materials where magnetism persists, it is unclear how the magnetic properties are affected. Here we study the evolution of the magnetic structure in Nd(1-x)Ce(x)CoIn(5) from the localized to the highly itinerant limit. We observe two magnetic ground states inside a heavy-fermion phase that are detached from unconventional superconductivity. The presence of two different magnetic phases provides evidence that increasing charge delocalization affects the magnetic interactions via anisotropic band hybridization.

cond-mat.str-el↗

arXiv2018

Total interference between nuclear and magnetovibrational one-phonon scattering cross sections

A full phonon intensity cancellation is reported in a longitudinal polarized inelastic neutron scattering experiment performed on the magnetocaloric compound MnFe$_{4}$Si$_{3}$, a ferromagnet with $T_{Curie}$ $\approx$ 305 K. The TA[100] phonon polarized along the $c$-axis measured from the Brillouin zone center $\textbf{G}$=(0, 0, 2) is observed only in one ($σ_{z}^{++}$) of the two non-spin-flip polarization channels and is absent in the other one ($σ_{z}^{--}$) at low temperatures. This effect disappears at higher temperatures, in the vicinity of $T_{Curie}$, where the phonon is measured in both channels with nonetheless marked different intensities. The effect is understood as originating from nuclear-magnetic interference between the nuclear one-phonon and the magnetovibrational one-phonon scattering cross-sections. The total cancellation reported is accidental, i.e. does not correspond to a systematic effect, as established by measurements in different Brillouin zones.

cond-mat.mtrl-sci↗

arXiv2018

Manifolds of magnetic ordered states and excitations in the almost Heisenberg pyrochlore antiferromagnet MgCr2O4

In spinels ACr2O4 (A=Mg, Zn) realisation of the classical pyrochlore Heisenberg antiferromagnet model is complicated by a strong spin-lattice coupling: the extensive degeneracy of the ground state is lifted by a magneto-structural transition at TN=12.5 K. We study the resulting low-temperature low-symmetry crystal structure by synchrotron x-ray diffraction. The consistent features of x-ray low-temperature patterns are explained by the tetragonal model of Ehrenberg et. al (Pow. Diff. 17, 230( 2002)), while other features depend on sample or cooling protocol. Complex partially ordered magnetic state is studied by neutron diffraction and spherical neutron polarimetry. Multiple magnetic domains of configuration arms of the propagation vectors k1=(1/2 1/2 0), k2=(1 0 1/2) appear. The ordered moment reaches 1.94(3) muB/Cr3+ for k1 and 2.08(3) muB/Cr3+ for k2, if equal amount of the k1 and k2 phases is assumed. The magnetic arrangements have the dominant components along the [110] and [1-10] diagonals and a smaller c-component. By inelastic neutron scattering we investigate the spin excitations, which comprise a mixture of dispersive spin waves propagating from the magnetic Bragg peaks and resonance modes centered at equal energy steps of 4.5 meV. We interpret these as acoustic and optical spin wave branches, but show that the neutron scattering cross sections of transitions within a unit of two corner-sharing tetrahedra match the observed intensity distribution of the resonances. The distinctive fingerprint of cluster-like excitations in the optical spin wave branches suggests that propagating excitations are localized by the complex crystal structure and magnetic orders.

cond-mat.str-el↗

arXiv2018

Spin-fluctuations drive the inverse magnetocaloric effect in Mn5Si3

Inelastic neutron scattering measurements were performed on single crystals of the antiferromagnetic compound Mn5Si3 in order to investigate the relation between the spin dynamics and the magneto-thermodynamic properties. It is shown that among the two stable antiferromagnetic phases of this compound, the high temperature one has an unusual magnetic excitation spectrum where propagative spin-waves and diffuse spin-fluctuations coexist. Moreover, it is evidenced that the inverse magnetocaloric effect of Mn5Si3, the cooling by adiabatic magnetization, is associated with field induced spin-fluctuations.

cond-mat.mtrl-sci↗

arXiv2018

Elastic softness of hybrid lead halide perovskites

Much recent attention has been devoted towards unravelling the microscopic optoelectronic properties of hybrid organic-inorganic perovskites (HOP). Here we investigate by coherent inelastic neutron scattering spectroscopy and Brillouin light scattering, low frequency acoustic phonons in four different hybrid perovskite single crystals: MAPbBr$_3$, FAPbBr$_3$, MAPbI$_3$ and $α$-FAPbI$_3$ (MA: methylammonium, FA: formamidinium). We report a complete set of elastic constants caracterized by a very soft shear modulus C$_{44}$. Further, a tendency towards an incipient ferroelastic transition is observed in FAPbBr$_3$. We observe a systematic lower sound group velocity in the technologically important iodide-based compounds compared to the bromide-based ones. The findings suggest that low thermal conductivity and hot phonon bottleneck phenomena are expected to be enhanced by low elastic stiffness, particularly in the case of the ultrasoft $α$-FAPbI$_3$.

cond-mat.mtrl-sci↗

arXiv2018

Distinct domain switching in Nd0.05Ce0.95CoIn5 at low and high fields

Nd0.05Ce0.95CoIn5 features a magnetic field-driven quantum phase transition that separates two antiferromagnetic phases with an identical magnetic structure inside the superconducting condensate. Using neutron diffraction we demonstrate that the population of the two magnetic domains in the two phases is affected differently by the rotation of the magnetic field in the tetragonal basal plane. In the low-field SDW-phase the domain population is only weakly affected while in the high-field Q-phase they undergo a sharp switch for fields around the a-axis. Our results provide evidence that the anisotropic spin susceptibility in both phases arises ultimately from spin-orbit interactions but are qualitatively different in the two phases. This provides evidence that the electronic structure is changed at the quantum phase transition, which yields a modified coupling between magnetism and superconductivity in the Q-phase.

cond-mat.str-el↗

arXiv2017

Topological quantum phase transition in the Ising-like antiferromagnetic spin chain BaCo$_2$V$_2$O$_8$

Since the seminal ideas of Berezinskii, Kosterlitz and Thouless, topological excitations are at the heart of our understanding of a whole novel class of phase transitions. In most of the cases, those transitions are controlled by a single type of topological objects. There are however some situations, still poorly understood, where two dual topological excitations fight to control the phase diagram and the transition. Finding experimental realization of such cases is thus of considerable interest. We show here that this situation occurs in BaCo$_2$V$_2$O$_8$, a spin-1/2 Ising-like quasi-one dimensional antiferromagnet when subjected to a uniform magnetic field transverse to the Ising axis. Using neutron scattering experiments, we measure a drastic modification of the quantum excitations beyond a critical value of the magnetic field. This quantum phase transition is identified, through a comparison with theoretical calculations, to be a transition between two different types of solitonic topological objects, which are captured by different components of the dynamical structure factor.

cond-mat.str-el↗

arXiv2017

Spin Resonance and Magnetic Order in an Unconventional Superconductor

Unconventional superconductivity in many materials is believed to be mediated by magnetic fluctuations. It is an open question how magnetic order can emerge from a superconducting condensate and how it competes with the magnetic spin resonance in unconventional superconductors. Here we study a model d-wave superconductor that develops spin-density wave order, and find that the spin resonance is unaffected by the onset of static magnetic order. This result suggests a scenario, in which the resonance in Nd0.05Ce0.95CoIn5 is a longitudinal mode with fluctuating moments along the ordered magnetic moments.

cond-mat.str-el↗

arXiv2017

Magnetic and dielectric order in the kagome-like francisite Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl

We report a single-crystal neutron diffraction and inelastic neutron scattering study on the spin 1/2 cuprate Cu$_3$Bi(SeO$_3$)$_2$O$_2$Cl, complemented by dielectric and electric polarization measurements. The study clarifies a number of open issues concerning this complex material, whose frustrated interactions on a kagome-like lattice, combined with Dzyaloshinskii-Moriya interactions, are expected to stabilize an exotic canted antiferromagnetic order. In particular, we determine the nature of the structural transition occurring at 115 K, the magnetic structure below 25 K resolved in the updated space group, and the microscopic ingredients at the origin of this magnetic arrangement. This was achieved by an analysis of the measured gapped spin waves, which signifies the need of an unexpected and significant anisotropic exchange beyond the proposed Dzyaloshinskii-Moriya interactions. Finally, we discuss the mutliferroic properties of this material with respect to the space group symmetries.

cond-mat.mtrl-sci↗

arXiv2015

Longitudinal and Transverse Zeeman Ladders in the Ising-Like Chain Antiferromagnet BaCo2V2O8

We explore the spin dynamics emerging from the Néel phase of the chain compound antiferromagnet BaCo2V2O8. Our inelastic neutron scattering study reveals unconventional discrete spin excitations, so called Zeeman ladders, understood in terms of spinon confinement, due to the interchain attractive linear potential. These excitations consist in two interlaced series of modes, respectively with transverse and longitudinal polarization. The latter have no classical counterpart and are related to the zero-point fluctuations that weaken the ordered moment in weakly coupled quantum chains. Our analysis reveals that BaCo2V2O8, with moderate Ising anisotropy and sizable interchain interactions, remarkably fulfills the conditions necessary for the observation of these longitudinal excitations.

cond-mat.str-el↗

arXiv2015

Ising incommensurate spin resonance of CeCoIn$_{5}$: a dynamical precursor of the Q-phase

It is shown by detailed inelastic neutron scattering experiments that the gapped collective magnetic excitation of the unconventional superconductor CeCoIn$_{5}$, the spin resonance mode, is incommensurate and that the corresponding fluctuations are of Ising nature. The incommensurate peak position of these fluctuations corresponds to the propagation vector of the adjacent field induced static magnetic ordered phase, the so-called Q-phase. Furthermore, the direction of the magnetic moment fluctuations is also the direction of the ordered magnetic moments of the Q-phase. Hence the resonance mode and the Q-phase share the same symmetry and this strongly supports a scenario where the static order is realized by a condensation of the magnetic excitation.

cond-mat.str-el↗

arXiv2014

Lattice dynamics of the heavy fermion compound URu$_2$Si$_2$

We report a comprehensive investigation of the lattice dynamics of URu$_2$Si$_2$ as a function of temperature using Raman scattering, optical conductivity and inelastic neutron scattering measurements as well as theoretical {\it ab initio} calculations. The main effects on the optical phonon modes are related to Kondo physics. The B$_{1g}$ ($Γ_3$ symmetry) phonon mode slightly softens below $\sim$100~K, in connection with the previously reported softening of the elastic constant, $C_{11}-C_{12}$, of the same symmetry, both observations suggesting a B$_{1g}$ symmetry-breaking instability in the Kondo regime. Through optical conductivity, we detect clear signatures of strong electron-phonon coupling, with temperature dependent spectral weight and Fano line shape of some phonon modes. Surprisingly, the line shapes of two phonon modes, E$_u$(1) and A$_{2u}$(2), show opposite temperature dependencies. The A$_{2u}$(2) mode loses its Fano shape below 150 K, whereas the E$_u$(1) mode acquires it below 100~K, in the Kondo cross-over regime. This may point out to momentum-dependent Kondo physics. By inelastic neutron scattering measurements, we have drawn the full dispersion of the phonon modes between 300~K and 2~K. No remarkable temperature dependence has been obtained including through the hidden order transition. {\it Ab initio} calculations with the spin-orbit coupling are in good agreement with the data except for a few low energy branches with propagation in the (a,b) plane.

cond-mat.str-el↗

arXiv2014

Magnetic-field enhanced aniferromagnetism in non-centrosymmetric heavy-fermion superconductor CePt$_3$Si

The effect of magnetic field on the static and dynamic spin correlations in the non-centrosymmetric heavy-fermion superconductor CePt$_3$Si was investigated by neutron scattering. The application of a magnetic field B increases the antiferromagnetic (AFM) peak intensity. This increase depends strongly on the field direction: for B${\parallel}$[0 0 1] the intensity increases by a factor of 4.6 at a field of 6.6 T, which corresponds to more than a doubling of the AFM moment, while the moment increases by only 10 % for B${\parallel}$[1 0 0] at 5 T. This is in strong contrast to the inelastic response near the antiferromagnetic ordering vector, where no marked field variations are observed for B${\parallel}$[0 0 1] up to 3.8 T. The results reveal that the AFM state in CePt$_3$Si, which coexists with superconductivity, is distinctly different from other unconventional superconductors.

cond-mat.str-el↗

arXiv2014

Switching of the magnetic order in CeRhIn$_{5-x}$Sn$_{x}$ in the vicinity of its quantum critical point

We report neutron diffraction experiments performed in the tetragonal antiferromagnetic heavy fermion system CeRhIn$_{5-x}$Sn$_{x}$ in its ($x$, $T$) phase diagram up to the vicinity of the critical concentration $x_c$ $\approx$ 0.40, where long range magnetic order is suppressed. The propagation vector of the magnetic structure is found to be $\bf{k_{IC}}$=(1/2, 1/2, $k_l$) with $k_l$ increasing from $k_l$=0.298 to $k_l$=0.410 when $x$ increases from $x$=0 to $x$=0.26. Surprisingly, for $x$=0.30, the order has changed drastically and a commensurate antiferromagnetism with $\bf{k_{C}}$=(1/2, 1/2, 0) is found. This concentration is located in the proximity of the quantum critical point where superconductivity is expected.

cond-mat.str-el↗

arXiv2013

Quantum criticality and Lifshitz transition in the Ising system CeRu2Si2: Comparison with YbRh2Si2

New thermoelectric power (TEP) measurements on prototype heavy-fermion compounds close to magnetic quantum criticality are presented. The highly sensitive technique of TEP is an unique tool to reveal Fermi surface instabilities, referred here as Lifshitz transitions. The first focus is on the Ising CeRu2Si2 series. Doping CeRu2Si2 with Rh produces a decoupling between the first order metamagnetic transition and the pseudo-metamagnetism observed in the pure compound. Comparison is made with the case of YbRh2Si2 which is often considered as the archetype of local quantum criticality by contrast to CeRu2Si2, taken as an example of spin-density wave criticality. Up to now for ferromagnetic materials showing ferromagnetic wings, no simple case appears where the Fermi surface is preserved between the ferromagnetic and paramagnetic phases. An open issue is the consequence of Lifshitz transitions on superconductivity in these multiband systems.

cond-mat.str-el↗

arXiv2013

Magnetic order in Ce0.95Nd0.05CoIn5: the Q-phase at zero magnetic field

We report neutron scattering experiment results revealing the nature of the magnetic order occurring in the heavy fermion superconductor Ce0.95Nd0.05CoIn5, a case for which an antiferromagnetic state is stabilized at a temperature below the superconducting transition one. We evidence an incommensurate order and its propagation vector is found to be identical to that of the magnetic field induced antiferromagnetic order occurring in the stoichiometric superconductor CeCoIn5, the so-called Q-phase. The commonality between these two cases suggests that superconductivity is a requirement for the formation of this kind of magnetic order and the proposed mechanism is the enhancement of nesting condition by d-wave order parameter with nodes in the nesting area.

cond-mat.str-el↗