Tuning the Multiferroic Properties of BiFeO_{3} under Uniaxial Strain.

More than twenty years ago, multiferroic compounds combining in particular magnetism and ferroelectricity were rediscovered. Since then, BiFeO_{3} has emerged as the most outstanding multiferroic by combining at room temperature almost all the fundamental or applicative properties that may be desired: electroactive spin wave excitations called electromagnons, conductive domain walls, or a low band gap of interest for magnonic devices. All these properties have so far only been discontinuously strain engineered in thin films according to the lattice parameter imposed by the substrate. Here we explore the ferroelectricity and the dynamic magnetic response of BiFeO_{3} bulk under continuously tunable uniaxial strain. Using elasto-Raman spectroscopy, we show that the ferroelectric soft mode is strongly enhanced under tensile strain and driven by the volume preserving deformation at low strain. The magnonic response is entirely modified with low energy magnon modes being suppressed for tensile strain above pointing out a transition from a cycloid to an homogeneous magnetic state. Effective Hamiltonian calculations show that the ferroelectric and the antiferrodistortive modes compete in the tensile regime. In addition, the homogeneous antiferromagnetic state becomes more stable compared to the cycloidal state above a +2% tensile strain close to the experimental value. Finally, we reveal the ferroelectric and magnetic orders of BiFeO_{3} under uniaxial strain and how the tensile strain allows us to unlock and to modify in a differentiated way the polarization and the magnetic structure.

Gate-Dependent Electronic Raman Scattering in Graphene.

We report the direct observation of polarization resolved electronic Raman scattering in a gated monolayer graphene device. The evolution of the electronic Raman scattering spectra with gate voltage and its polarization dependence are in full agreement with theoretical expectations for nonresonant Raman processes involving interband electron-hole excitations across the Dirac cone. We further show that the spectral dependence of the electronic Raman scattering signal can be simply described by the dynamical polarizability of graphene in the long wavelength limit. The possibility to directly observe Dirac fermion excitations in graphene opens the way to promising Raman investigations of electronic properties of graphene and other 2D crystals.

Unconventional High-Energy-State Contribution to the Cooper Pairing in the Underdoped Copper-Oxide Superconductor HgBa_{2}Ca_{2}Cu_{3}O_{8+δ}.

We study the temperature-dependent electronic B_{1g} Raman response of a slightly underdoped single crystal HgBa_{2}Ca_{2}Cu_{3}O_{8+δ} with a superconducting critical temperature T_{c}=122 K. Our main finding is that the superconducting pair-breaking peak is associated with a dip on its higher-energy side, disappearing together at T_{c}. This result reveals a key aspect of the unconventional pairing mechanism: spectral weight lost in the dip is transferred to the pair-breaking peak at lower energies. This conclusion is supported by cellular dynamical mean-field theory on the Hubbard model, which is able to reproduce all the main features of the B_{1g} Raman response and explain the peak-dip behavior in terms of a nontrivial relationship between the superconducting gap and the pseudogap.

Driving Spin Excitations by Hydrostatic Pressure in BiFeO(3).

Optical spectroscopy has been combined with computational and theoretical techniques to show how the spin dynamics in the model multiferroic BiFeO(3) responds to the application of hydrostatic pressure and its corresponding series of structural phase transitions from R3c to the Pnma phases. As pressure increases, multiple spin excitations associated with noncollinear cycloidal magnetism collapse into two excitations, which show jump discontinuities at some of the ensuing crystal phase transitions. The effective Hamiltonian approach provides information on the electrical polarization and structural changes of the oxygen octahedra through the successive structural phases. The extracted parameters are then used in a Ginzburg-Landau model to reproduce the evolution with pressure of the spin wave excitations observed at low energy, and we demonstrate that the structural phases and the magnetic anisotropy drive and control the spin excitations.

Collapse of the normal-state pseudogap at a Lifshitz transition in the Bi(2)Sr(2)CaCu(2)O(8+δ) cuprate superconductor.

We report a fine tuned doping study of strongly overdoped Bi_{2}Sr_{2}CaCu_{2}O_{8+δ} single crystals using electronic Raman scattering. Combined with theoretical calculations, we show that the doping, at which the normal-state pseudogap closes, coincides with a Lifshitz quantum phase transition where the active holelike Fermi surface becomes electronlike. This conclusion suggests that the microscopic cause of the pseudogap is sensitive to the Fermi surface topology. Furthermore, we find that the superconducting transition temperature is unaffected by this transition, demonstrating that their origins are different on the overdoped side.

Crafting the magnonic and spintronic response of BiFeO3 films by epitaxial strain.

Multiferroics are compounds that show ferroelectricity and magnetism. BiFeO3, by far the most studied, has outstanding ferroelectric properties, a cycloidal magnetic order in the bulk, and many unexpected virtues such as conductive domain walls or a low bandgap of interest for photovoltaics. Although this flurry of properties makes BiFeO3 a paradigmatic multifunctional material, most are related to its ferroelectric character, and its other ferroic property--antiferromagnetism--has not been investigated extensively, especially in thin films. Here we bring insight into the rich spin physics of BiFeO3 in a detailed study of the static and dynamic magnetic response of strain-engineered films. Using Mössbauer and Raman spectroscopies combined with Landau-Ginzburg theory and effective Hamiltonian calculations, we show that the bulk-like cycloidal spin modulation that exists at low compressive strain is driven towards pseudo-collinear antiferromagnetism at high strain, both tensile and compressive. For moderate tensile strain we also predict and observe indications of a new cycloid. Accordingly, we find that the magnonic response is entirely modified, with low-energy magnon modes being suppressed as strain increases. Finally, we reveal that strain progressively drives the average spin angle from in-plane to out-of-plane, a property we use to tune the exchange bias and giant-magnetoresistive response of spin valves.

Symmetry of the excitations in the hidden order state of URu2Si2.

We perform polarized electronic Raman scattering on URu2Si2 single crystals at low temperature down to 8 K in the hidden-order state and under a magnetic field up to 10 T. The hidden-order state is characterized by a sharp excitation at 1.7 meV and a gap in the electronic continuum below 6.8 meV. Both Raman signatures are of pure A2g symmetry. By comparing the behavior of the Raman sharp excitation and the neutron resonance at Q0=(0,0,1), we provide new evidence, constrained by selection rules of the two probes, that the hidden-order state breaks the translational symmetry along the c axis such that Γ and Z points fold on top of each other. The observation of these distinct Raman features with a peculiar A2g symmetry as a signature of the hidden-order phase places strong constraints on current theories of the hidden-order in URu2Si2.

New insights into the phase diagram of the copper oxide superconductors from electronic Raman scattering.

The mechanism of unconventional superconductivity is still unknown despite over 25 years passing since the discovery of high-T(c) cuprate superconductors by Bednorz and Muller (1986 Z. Phys. B 64 189). Here, we explore the cuprate phase diagram by electronic Raman spectroscopy and shed light on the superconducting state in hole-doped curates, namely, how superconductivity and the critical temperature T(c) are affected by the pseudogap.

Observation of incipient charge nematicity in Ba(Fe(1-x)Co(x))2As2.

Using electronic Raman spectroscopy, we report direct measurements of charge nematic fluctuations in the tetragonal phase of strain-free Ba(Fe(1-x)Co(x))2As2 single crystals. The strong enhancement of the Raman response at low temperatures unveils an underlying charge nematic state that extends to superconducting compositions and which has hitherto remained unnoticed. Comparison between the extracted charge nematic susceptibility and the elastic modulus allows us to disentangle the charge contribution to the nematic instability, and to show that charge nematic fluctuations are weakly coupled to the lattice.

Raman-scattering measurements and theory of the energy-momentum spectrum for underdoped Bi2Sr2CaCuO(8+δ) superconductors: evidence of an s-wave structure for the pseudogap.

We reveal the full energy-momentum structure of the pseudogap of underdoped high-Tc cuprate superconductors. Our combined theoretical and experimental analysis explains the spectral-weight suppression observed in the B2g Raman response at finite energies in terms of a pseudogap appearing in the single-electron excitation spectra above the Fermi level in the nodal direction of momentum space. This result suggests an s-wave pseudogap (which never closes in the energy-momentum space), distinct from the d-wave superconducting gap. Recent tunneling and photoemission experiments on underdoped cuprates also find a natural explanation within the s-wave pseudogap scenario.

Electric-field control of spin waves at room temperature in multiferroic BiFeO3.

To face the challenges lying beyond present technologies based on complementary metal-oxide-semiconductors, new paradigms for information processing are required. Magnonics proposes to use spin waves to carry and process information, in analogy with photonics that relies on light waves, with several advantageous features such as potential operation in the terahertz range and excellent coupling to spintronics. Several magnonic analog and digital logic devices have been proposed, and some demonstrated. Just as for spintronics, a key issue for magnonics is the large power required to control/write information (conventionally achieved through magnetic fields applied by strip lines, or by spin transfer from large spin-polarized currents). Here we show that in BiFeO(3), a room-temperature magnetoelectric material, the spin-wave frequency (>600 GHz) can be tuned electrically by over 30%, in a non-volatile way and with virtually no power dissipation. Theoretical calculations indicate that this effect originates from a linear magnetoelectric effect related to spin-orbit coupling induced by the applied electric field. We argue that these properties make BiFeO(3) a promising medium for spin-wave generation, conversion and control in future magnonics architectures.

Magnetic field induced dehybridization of the electromagnons in multiferroic TbMnO3.

We have studied the impact of the magnetic field on the electromagnon excitations in TbMnO3 crystal. Applying a magnetic field along the c axis, we show that the electromagnons transform into pure antiferromagnetic modes, losing their polar character. Entering in the paraelectric phase, we are able to track the spectral weight transfer from the electromagnons to the magnon excitations and we discuss the magnetic excitations underlying the electromagnons. We also point out the phonons involved in the phase transition process. This reveals that the Mn-O distance plays a key role in understanding the ferroelectricity and the polar character of the electromagnons. Magnetic field measurements along the b axis allow us to detect a new electromagnon resonance in agreement with a Heisenberg model.

Possible observation of the signature of the bad metal phase and its crossover to a Fermi liquid in κ-(BEDT-TTF)2Cu(NCS)2 bulk and nanoparticles by Raman scattering.

κ-(BEDT-TTF)2Cu(NCS)2 has been investigated by Raman scattering in both bulk and nanoparticle compounds. Phonon modes from 20 to 1600 cm-1 have been assigned. Focusing on the unexplored low frequency phonons, a plateau in frequencies is observed in the bulk phonons between 50 and 100 K and assigned to the signature of the bad metal phase. Nanoparticles of κ-(BEDT-TTF)2Cu(NCS)2 exhibit anomalies at 50 K associated to the crossover from a bad metal to a Fermi liquid whose origins are discussed.

Elastic and magnetoelastic properties of TbMnO3single crystal by nanosecond time resolved acoustics and first-principles calculations.

Time resolved pump and probe acoustics and first-principles calculations were employed to assess elastic properties of the TbMnO3perovskite manganite having orthorhombic symmetry. Measuring sound velocities of bulk longitudinal and shear acoustic waves propagating along at least two different directions in the high symmetry planes (100), (010) and (001), provided a powerful mean to selectively determine the six diagonal elastic constantsC11= 227 GPa,C22= 349 GPa,C33= 274 GPa,C44= 71 GPa,C55= 57 GPa,C66= 62 GPa. Among the three remaining off-diagonal ones,C23= 103 GPa was determined with a bissectrice direction. Density functional theory calculations with colinear spin-polarized provided complementary insights on their optical, elastic and magnetoelastic properties.

Nematic fluctuations in the cuprate superconductor Bi2Sr2CaCu2O8+δ.

Establishing the presence and the nature of a quantum critical point in their phase diagram is a central enigma of the high-temperature superconducting cuprates. It could explain their pseudogap and strange metal phases, and ultimately their high superconducting temperatures. Yet, while solid evidences exist in several unconventional superconductors of ubiquitous critical fluctuations associated to a quantum critical point, in the cuprates they remain undetected until now. Here using symmetry-resolved electronic Raman scattering in the cuprate [Formula: see text], we report the observation of enhanced electronic nematic fluctuations near the endpoint of the pseudogap phase. While our data hint at the possible presence of an incipient nematic quantum critical point, the doping dependence of the nematic fluctuations deviates significantly from a canonical quantum critical scenario. The observed nematic instability rather appears to be tied to the presence of a van Hove singularity in the band structure.

Strain and Magnetic Field Induced Spin-Structure Transitions in Multiferroic BiFeO3.

The magnetic-field-dependent spin ordering of strained BiFeO3 films is determined using nuclear resonant scattering and Raman spectroscopy. The critical field required to destroy the cycloidal modulation of the Fe spins is found to be significantly lower than in the bulk, with appealing implications for field-controlled spintronic and magnonic devices.

Control of ferroelectricity and magnetism in multi-ferroic BiFeO3 by epitaxial strain.

Recently, strain engineering has been shown to be a powerful and flexible means of tailoring the properties of ABO3 perovskite thin films. The effect of epitaxial strain on the structure of the perovskite unit cell can induce a host of interesting effects, these arising from either polar cation shifts or rotation of the oxygen octahedra, or both. In the multi-ferroic perovskite bismuth ferrite (BiFeO3-BFO), both degrees of freedom exist, and thus a complex behaviour may be expected as one plays with epitaxial strain. In this paper, we review our results on the role of strain on the ferroic transition temperatures and ferroic order parameters. We find that, while the Néel temperature is almost unchanged by strain, the ferroelectric Curie temperature strongly decreases as strain increases in both the tensile and compressive ranges. Also unexpected is the very weak influence of strain on the ferroelectric polarization value. Using effective Hamiltonian calculations, we show that these peculiar behaviours arise from the competition between antiferrodistortive and polar instabilities. Finally, we present results on the magnetic order: while the cycloidal spin modulation present in the bulk survives in weakly strained films, it is destroyed at large strain and replaced by pseudo-collinear antiferromagnetic ordering. We discuss the origin of this effect and give perspectives for devices based on strain-engineered BiFeO3.

Possible observation of cycloidal electromagnons in BiFeO3.

We unravel the magnon spectra of BiFeO3 by means of low-energy inelastic light scattering. We show the existence of two species of magnons corresponding to spin wave excitations in and out of the cycloidal plane. These excitations might be interpreted as electromagnon modes. The present observations present an unique opportunity to study the competition between ferroelectric and magnetic orders.

Temperature dependence of the gap size near the brillouin-zone nodes of HgBa2CuO4+delta superconductors.

Although more than 20 years have passed, the identification of the superconducting order parameter in cuprates is still under debate. Here, we show that the gap size near the nodes is a good candidate for the order parameter: it scales with the critical temperature Tc over a wide doping range and displays a significant temperature dependence below Tc in both the underdoped and the overdoped regimes. In contrast, the gap size at the antinodes does not scale with Tc in the underdoped regime and appears to be controlled by the pseudogap which persists below Tc.

Intrinsic low temperature paramagnetism in B-DNA.

We present an experimental study of magnetization in lambda-DNA in conjunction with structural measurements. The results show the surprising interplay between the molecular structures and their magnetic property. In the B-DNA state, lambda-DNA exhibits paramagnetic behavior below 20 K that is nonlinear in an applied magnetic field whereas, in the A-DNA state, it remains diamagnetic down to 2 K. We propose orbital paramagnetism as the origin of the observed phenomena and discuss its relation to the existence of long range coherent transport in B-DNA at low temperature.