arXiv subjects

S. Petit

Publications and source records attributed to S. Petit.

At least 55 records · Page 3Linked to original sources

arXiv2015

Fluctuations and all-in$-$all-out ordering in dipole-octupole Nd2Zr2O7

We present an experimental study of the pyrochlore coumpound Nd2Zr2O7 by means of neutron scattering and magnetization measurements down to 90 mK. The Nd$^{3+}$ magnetic moments exhibit a strong local $\langle$111$\rangle$ Ising anisotropy together with a dipolar-octupolar nature, different from the standard Kramers-doublet studied so far. We show that, despite the positive Curie-Weiss temperature, \ndzr\ undergoes a transition around 285 mK towards an all-in$-$all-out antiferromagnetic state. We establish the $(H,T)$ phase diagram in the three directions of the applied field and reveal a metamagnetic transition around 0.1 T. The strongly reduced ordered magnetic moment as well as the unexpected shape of the magnetization curves demonstrate that Nd2Zr2O7 , is not a standard Ising antiferromagnet. We propose that the peculiar nature of the Nd doublet combined with competing interactions explain these findings.

cond-mat.str-el↗

arXiv2015

Spin dynamics in the presence of competing ferro- and antiferro-magnetic correlations in Yb2Ti2O7

In this work, we show that the zero field excitation spectra in the quantum spin ice candidate pyrochlore compound \ybti\ is a continuum characterized by a very broad and almost flat dynamical response which extends up to $1-1.5$ meV, coexisting or not with a quasi-elastic response depending on the wave-vector. The spectra do not evolve between 50 mK and 2 K, indicating that the spin dynamics is only little affected by the temperature in both the short-range correlated and ordered regimes. Although classical spin dynamics simulations qualitatively capture some of the experimental observations, we show that they fail to reproduce this broad continuum. In particular, the simulations predict an energy scale twice smaller than the experimental observations. This analysis is based on a careful determination of the exchange couplings, able to reproduce both the zero field diffuse scattering and the spin wave spectrum rising in the field polarized state. According to this analysis, \ybti\ lies at the border between a ferro and an antiferromagnetic phase. These results suggest that the unconventional ground state of \ybti\ is governed by strong quantum fluctuations arising from the competition between those phases. The observed spectra may correspond to a continuum of deconfined spinons as expected in quantum spin liquids.

cond-mat.str-el↗

arXiv2014

Order by Disorder and Energetic Selection of the Ground State in the XY Pyrochlore Antiferromagnet Er2Ti2O7. An Inelastic Neutron Scattering Study

Examples of materials where an "order by disorder" mechanism is at play to select a particular ground state are scarce. It has recently been proposed, however, that the antiferromagnetic XY pyrochlore Er2Ti2O7, reveals a most convincing case of this mechanism. Observation of a spin gap at zone centers has recently been interpreted as a corroboration of this physics. In this paper, we argue, however, that the anisotropy generated by the interaction-induced admixing between the crystal-field ground and excited levels provides for an alternative mechanism. It especially predicts the opening of a spin gap of about 15 micro-eV, which is of the same order of magnitude as the one observed experimentally. We report new high resolution inelastic neutron scattering data which can be well understood within this scenario.

cond-mat.str-el↗

arXiv2014

Temperature-Dependent Interplay of Dzyaloshinskii-Moriya Interaction and Single-Ion Anisotropy in Multiferroic BiFeO$_3$

Low-energy magnon excitations in multiferroic BiFeO$_3$ were measured in detail as a function of temperature around several Brillouin zone centers by inelastic neutron scattering experiments on single crystals. Unique features around 1 meV are directly associated with the interplay of the Dzyaloshinskii-Moriya interaction and a small single-ion anisotropy. The temperature dependence of these and the exchange interactions were determined by fitting the measured magnon dispersion with spin-wave calculations. The spectra best fits an easy-axis type magnetic anisotropy and the deduced exchange and anisotropy parameters enable us to determine the anharmonicity of the magnetic cycloid. We then draw a direct connection between the changes in the parameters of spin Hamiltonian with temperature and the physical properties and structural deformations of BiFeO$_3$.

cond-mat.mtrl-sci↗

arXiv2014

Multi-channel Electronic and Vibrational Dynamics in Polyatomic High-order Harmonic Generation

High-order harmonic generation in polyatomic molecules generally involves multiple channels, each associated with a different orbital. Their unambiguous assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach, using unaligned SF$_6$ molecules as an example, where we combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Channel-resolved above-threshold ionization measurements reveal that strong-field ionization opens four channels. Two of them, identified by monitoring the ellipticity dependence of the high-harmonic emission, are found to dominate the harmonic signal. A switch from the HOMO-3 to the HOMO-1 channel at 26 eV is confirmed by a phase jump in the harmonic emission, and by the differing dynamical responses to molecular vibrations. This study demonstrates a modus operandi for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected.

physics.chem-ph↗

arXiv2014

Lattice and spin excitations in multiferroic h-YMnO3

We used Raman and terahertz spectroscopies to investigate lattice and magnetic excitations and their cross-coupling in the hexagonal YMnO3 multiferroic. Two phonon modes are strongly affected by the magnetic order. Magnon excitations have been identified thanks to comparison with neutron measurements and spin wave calculations but no electromagnon has been observed. In addition, we evidenced two additional Raman active peaks. We have compared this observation with the anti-crossing between magnon and acoustic phonon branches measured by neutron. These optical measurements underly the unusual strong spin-phonon coupling.

cond-mat.str-el↗

arXiv2013

Low temperature diffuse neutron scattering and magnetisation in single crystal Tb2Ti2O7

We present an interpretation of zero field diffuse neutron scattering and of high field magnetisation data at very low temperature in the frustrated pyrochlore system Tb2Ti2O7. This material has antiferromagnetic exchange interactions and it is expected to have Ising character at low temperature. Contrary to expectations, it shows no magnetic ordering down to 0.05\,K, being thus labelled a "spin liquid". However, the ground state in Tb2Ti2O7 is not a mere fluctuating moment paramagnet but, as demonstrated by very recent experiments, a state where the electronic degrees of freedom are hybridised with the phononic variables in an unconventional way. We show here that, by approximating this complex and still unraveled electron-phonon interaction by a dynamic Jahn-Teller coupling, one can account rather well for the diffuse neutron scattering and the low temperature isothermal magnetisation. We discuss the shortcomings of this picture which arise mainly from the fact that the singlet electronic mean field ground state of the model fails to reproduce the observed strong intensity of the elastic and quasi-elastic neutron scattering.

cond-mat.str-el↗

arXiv2013

An ab initio study of magneto-electric coupling of $\rm YMnO_3$

The present paper proposes the direct calculation of the microscopic contributions to the magneto-electric coupling, using ab initio methods. The electrostrictive and the Dzyaloshinskii-Moriya contributions were evaluated individually. For this purpose a specific method was designed, combining DFT calculations and embedded fragments, explicitely correlated, quantum chemical calculations. This method allowed us to calculate the evolution of the magnetic couplings as a function of an applied electric field. We found that in $\rm YMnO_3$ the Dzyaloshinskii-Moriya contribution to the magneto-electric effect is three orders of magnitude weaker than the electrostrictive contribution. Strictive effects are thus dominant in the magnetic exchange evolution under an applied electric field, and by extension on the magneto-electric effect. These effects remain however quite small and the modifications of the magnetic excitations under an applied electric field will be difficult to observe experimentally. Another important conclusion is that the amplitude of the magneto-electric effect is very small. Indeed, it can be shown that the linear magneto-electric tensor is null due to the inter-layer symmetry operations.

cond-mat.str-el↗

arXiv2013

Low temperature structural effects in the (TMTSF)$_2$PF$_6$ and AsF$_6$ Bechgaard salts

We present a detailed low-temperature investigation of the statics and dynamics of the anions and methyl groups in the organic conductors (TMTSF)$_2$PF$_6$ and (TMTSF)$_2$AsF$_6$ (TMTSF : tetramethyl-tetraselenafulvalene). The 4 K neutron scattering structure refinement of the fully deuterated (TMTSF)$_2$PF$_6$-D12 salt allows locating precisely the methyl groups at 4 K. This structure is compared to the one of the fully hydrogenated (TMTSF)$_2$PF$_6$-H12 salt previously determined at the same temperature. Surprisingly it is found that deuteration corresponds to the application of a negative pressure of 5 x 10$^2$ MPa to the H12 salt. Accurate measurements of the Bragg intensity show anomalous thermal variations at low temperature both in the deuterated PF$_6$ and AsF$_6$ salts. Two different thermal behaviors have been distinguished. Low-Bragg-angle measurements reflect the presence of low-frequency modes at characteristic energies θ$_E$ = 8.3 K and θ$_E$ = 6.7 K for the PF$_6$-D12 and AsF$_6$-D12 salts, respectively. These modes correspond to the low-temperature methyl group motion. Large-Bragg-angle measurements evidence an unexpected structural change around 55 K which probably corresponds to the linkage of the anions to the methyl groups via the formation of F...D-CD2 bonds observed in the 4 K structural refinement. Finally we show that the thermal expansion coefficient of (TMTSF)$_2$PF$_6$ is dominated by the librational motion of the PF$_6$ units. We quantitatively analyze the low-temperature variation of the lattice expansion via the contribution of Einstein oscillators, which allows us to determine for the first time the characteristic frequency of the PF6 librations: θ$_E$ = 50 K and θ$_E$ = 76 K for the PF$_6$-D12 and PF$_6$-H12 salts, respectively.

cond-mat.str-el↗

arXiv2013

Inhomogeneous High-order Harmonic Generation in Krypton Clusters

High order harmonic generation from clusters is a controversial topic: conflicting theories exist, with different explanations for similar experimental observations. From an experimental point of view, separating the contributions from monomers and clusters is challenging. By performing a spectrally and spatially resolved study in a controlled mixture of clusters and monomers, we are able to isolate a region of the spectrum where the emission purely originates from clusters. Surpringly, the emission from clusters is depolarized, which is the signature of statistical inhomogeneous emission from a low-density source. The harmonic response to laser ellipticity shows that this generation is produced by a new recollisional mechanism, which opens the way to future theoretical studies.

physics.atm-clus↗

arXiv2013

Role of the Ionic Potential in High Harmonic Generation

Recollision processes provide direct insight into the structure and dynamics of electronic wave functions. However, the strength of the process sets its basic limitations - the interaction couples numerous degrees of freedom. In this Letter we decouple the basic steps of the process and resolve the role of the ionic potential which is at the heart of a broad range of strong field phenomena. Specifically, we measure high harmonic generation from argon atoms. By manipulating the polarization of the laser field we resolve the vectorial properties of the interaction. Our study shows that the ionic core plays a significant role in all steps of the interaction. In particular, Coulomb focusing induces an angular deflection of the electrons before recombination. A complete spatiospectral analysis reveals the influence of the potential on the spatiotemporal properties of the emitted light.

physics.atom-ph↗

arXiv2012

High-harmonic transient grating spectroscopy of NO2 electronic relaxation

We study theoretically and experimentally the electronic relaxation of NO2 molecules excited by absorption of one ~400 nm pump photon. Semi-classical simulations based on trajectory surface hopping calculations are performed. They predict fast oscillations of the electronic character around the intersection of the ground and first excited diabatic states. An experiment based on high-order harmonic transient grating spectroscopy reveals dynamics occuring on the same timescale. A systematic study of the detected transient is conducted to investigate the possible influence of the pump intensity, pump wavelength, and rotational temperature of the molecules. The quantitative agreement between measured and predicted dynamics shows that, in NO2, high harmonic transient grating spectroscopy encodes vibrational dynamics underlying the electronic relaxation.

physics.chem-ph↗

arXiv2011

Role of Antisymmetric Exchange in Selecting Magnetic Chirality in Ba$_3$NbFe$_3$Si$_2$O$_{14}$

We present electron spin resonance (ESR) investigation of the acentric \FeLang, featuring a unique single-domain double-chiral magnetic ground state. Combining simulations of the ESR line-width anisotropy and the antiferromagnetic-resonance modes allows us to single out the Dzyaloshinsky-Moriya (DM) interaction as the leading magnetic anisotropy term. We demonstrate that the rather minute out-of-plane DM component $d_c=45$ mK is responsible for selecting a unique ground state, which endures thermal fluctuations up to astonishingly high temperatures.

cond-mat.str-el↗

arXiv2011

InMnO3 : a fully frustrated multiferroic

InMnO$_3$ is a peculiar member of the hexagonal manganites h-RMnO$_3$ (where R is a rare earth metal element), showing crystalline, electronic and magnetic properties at variance with the other compounds of the family. We have studied high quality samples synthesized at high pressure and temperature by powder neutron diffraction. The position of the Mn ions is found to be close to the threshold $\it{x}=1/3$ where superexchange Mn-Mn interactions along the $\it{c}$ axis compensate. Magnetic long range order occurs below $T_{\rm N}$= 120(2) K with a magnetic unit cell doubled along $\it{c}$, whereas short range two dimensional dynamical spin correlations are observed above $T_{\rm N}$. We propose that pseudo-dipolar interactions are responsible for the long period magnetic structure.

cond-mat.mtrl-sci↗

arXiv2011

Tb$_2$Ti$_2$O$_7$, a two singlet spin-liquid pyrochlore

The pyrochlore compound \tbti\ is known to remain in a spin-liquid state down to the lowest attainable temperature (0.05\,K), whereas current theories predict it should order into an antiferromagnetic structure. A number of models have been developed in order to resolve this discrepancy, but they could not obtain a spin-liquid ground state. We present here an explanation for the lack of magnetic order in \tbti\ based on the presence of a Jahn-Teller-like distortion from the local trigonal symmetry and on the physics of the two-singlet system coupled by exchange.

cond-mat.str-el↗

arXiv2010

High-order Harmonic Spectroscopy of the Cooper Minimum in Argon: Experimental and Theoretical Study

We study the Cooper minimum in high harmonic generation from argon atoms using long wavelength laser pulses. We find that the minimum in high harmonic spectra is systematically shifted with respect to total photoionization cross section measurements. We use a semi-classical theoretical approach based on Classical Trajectory Monte Carlo and Quantum Electron Scattering methods (CTMC-QUEST) to model the experiment. Our study reveals that the shift between photoionization and high harmonic emission is due to several effects: the directivity of the recombining electrons and emitted polarization, and the shape of the recolliding electron wavepacket.

physics.atom-ph↗

arXiv2010

Two- and three-dimensional magnetic correlations in the spin-1/2 square-lattice system Zn2VO(PO4)2

The magnetic correlations in the quasi-two dimensional spin-1/2 square-lattice system Zn2VO(PO4)2 have been investigated by neutron diffraction technique. A long-range antiferromagnetic (AFM) ordering below 3.75 K (TN) has been observed with a reduced moment of 0.66(2) μB per V ion at 1.5 K. In a given ab plane, the AFM spin arrangement is Néel type and the AFM layers are coupled ferromagnetically along the c axis. Remarkably, we have observed a pure 2D short-range AFM ordering in the ab plane above TN. Interestingly, the coexistence of diffuse magnetic scattering and three dimensional antiferromagnetic Bragg peaks has been found below TN, indicating the presence of spin-waves as confirmed by our calculation using the linear spin-wave theory. The observed results are discussed in the light of existing theory for a two-dimensional spin-1/2 square-lattice system.

cond-mat.mtrl-sci↗

arXiv2009

Spin dynamics in the geometrically frustrated multiferroic CuCrO2

The spin dynamics of the geometrically frustrated triangular antiferromagnet multiferroic CuCrO2 have been mapped out using inelastic neutron scattering. The relevant spin Hamiltonian parameters modelling the incommensurate modulated helicoid have been determined, and correspond to antiferromagnetic nearest and next-nearest neighbour interactions in the ab plane, with a strong planar anisotropy. The weakly dispersive excitation along c reflects the essentially two-dimensional character of the magnetic interactions and according to classical energy calculations it is weakly ferromagnetic. Our results clearly point out the relevance of the balance between a ferromagnetic coupling between adjacent planes and a weakly antiferromagnetic next-nearest neighbour interaction in stabilising the three-dimensional ferroelectric magnetic order in CuCrO2. This novel insight on the interplay between magnetic interactions in CuCrO2 should provide a useful basis in the design of new delafossite-based multiferroic materials.

cond-mat.str-el↗