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U. Staub

Publications and source records attributed to U. Staub.

At least 37 records · Page 2Linked to original sources

Crystal Symmetry Lowering in Chiral Multiferroic Ba$_3$TaFe$_3$Si$_2$O$_{14}$ observed by X-Ray Magnetic Scattering

Chiral multiferroic langasites have attracted attention due to their doubly-chiral magnetic ground state within an enantiomorphic crystal. We report on a detailed resonant soft X-ray diffraction study of the multiferroic Ba$_3$TaFe$_3$Si$_2$O$_{14}$ at the Fe $L_{2,3}$ and oxygen $K$ edges. Below $T_N$ ($\approx27K$) we observe the satellite reflections $(0,0,τ)$, $(0,0,2τ)$, $(0,0,3τ)$ and $(0,0,1-3τ)$ where $τ\approx 0.140 \pm 0.001$. The dependence of the scattering intensity on X-ray polarization and azimuthal angle indicate that the odd harmonics are dominated by the out-of-plane ($\mathbf{\hat{c}}$-axis) magnetic dipole while the $(0,0,2τ)$ originates from the electron density distortions accompanying magnetic order. We observe dissimilar energy dependences of the diffraction intensity of the purely magnetic odd-harmonic satellites at the Fe $L_3$ edge. Utilizing first-principles calculations, we show that this is a consequence of the loss of threefold crystal symmetry in the multiferroic phase.

cond-mat.str-el↗

Magnetic properties of strained multiferroic CoCr2O4: a soft X-ray study

Using resonant soft X-ray techniques we follow the magnetic behavior of a strained epitaxial film of CoCr2O4, a type-II multiferroic. The film is [110]-oriented, such that both the ferroelectric and ferromagnetic moments can coexist in plane. X-ray magnetic circular dichroism (XMCD) is used in scattering and in transmission modes to probe the magnetization of Co and Cr separately. The transmission measurements utilized X-ray excited optical luminescence from the substrate. Resonant soft X-ray diffraction (RSXD) was used to study the magnetic order of the low temperature phase. The XMCD signals of Co and Cr appear at the same ordering temperature Tc~90K, and are always opposite in sign. The coercive field of the Co and of Cr moments is the same, and is approximately two orders of magnitude higher than in bulk. Through sum rules analysis an enlarged Co2+ orbital moment (m_L) is found, which can explain this hardening. The RSXD signal of the (q q 0) reflection appears below Ts, the same ordering temperature as the conical magnetic structure in bulk, indicating that this phase remains multiferroic under strain. To describe the azimuthal dependence of this reflection, a slight modification is required to the spin model proposed by the conventional Lyons-Kaplan-Dwight-Menyuk theory for magnetic spinels. Lastly, a slight increase in reflected intensity is observed below Ts=27K when measuring at the Cr edge (but not at the Co edge).

cond-mat.str-el↗

Nonlinear electron-phonon coupling in doped manganites

We employ time-resolved resonant x-ray diffraction to study the melting of charge order and the associated insulator-metal transition in the doped manganite Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ after resonant excitation of a high-frequency infrared-active lattice mode. We find that the charge order reduces promptly and highly nonlinearly as function of excitation fluence. Density functional theory calculations suggest that direct anharmonic coupling between the excited lattice mode and the electronic structure drive these dynamics, highlighting a new avenue of nonlinear phonon control.

cond-mat.str-el↗

Multiferroic properties of uniaxially compressed orthorhombic HoMnO3 thin films

Multiferroic properties of orthorhombic HoMnO3 (Pbnm space group) are significantly modified by epitaxial compressive strain along the a-axis. We are able to focus on the effect of strain solely along the a-axis by using an YAlO3 (010) substrate, which has only a small lattice mismatch with HoMnO3 along the other in-plane direction (the c-axis). Multiferroic properties of strained and relaxed HoMnO3 thin films are compared with those reported for bulk, and are found to differ widely. A relaxed film exhibits bulk-like properties such as a ferroelectric transition temperature of 25 K and an incommensurate antiferromagnetic order below 39 K, with an ordering wave vector of (0 qb 0) with qb ~ 0.41 at 10 K. A strained film becomes ferroelectric already at 37.5 K and has an incommensurate magnetic order with qb ~ 0.49 at 10 K.

cond-mat.mtrl-sci↗

Quasi-static magnetoelectric quadrupoles as the order parameter for the pseudo-gap phase in cuprate superconductors

We introduce a mechanism in which coupling between fluctuating spin magnetic dipole moments and polar optical phonons leads to a non-zero ferroic ordering of quasi-static magnetoelectric multipoles. Using first-principles calculations within the LSDA$+U$ method of density functional theory, we calculate the magnitude of the effect for the prototypical cuprate superconductor, HgBa$_2$CuO$_4$. We show that our proposed mechanism is consistent, to our knowledge, with all experimental data for the onset of the pseudo-gap phase and therefore propose the quasi-static magnetoelectric multipole as a possible pseudo-gap order parameter. Finally, we show that our mechanism embraces some key aspects of previous theoretical models, in particular the description of the pseudo-gap phase in terms of orbital currents.

cond-mat.supr-con↗

Itinerant and localized magnetization dynamics in antiferromagnetic Ho

Using femtosecond time-resolved resonant magnetic x-ray diffraction at the Ho L3 absorption edge, we investigate the demagnetization dynamics in antiferromagnetically ordered metallic Ho after femtosecond optical excitation. Tuning the x-ray energy to the electric dipole (E1, 2p -> 5d) or quadrupole (E2, 2p -> 4f) transition allows us to selectively and independently study the spin dynamics of the itinerant 5d and localized 4f electronic subsystems via the suppression of the magnetic (2 1 3-tau ) satellite peak. We find demagnetization timescales very similar to ferromagnetic 4f systems, suggesting that the loss of magnetic order occurs via a similar spin-flip process in both cases. The simultaneous demagnetization of both subsystems demonstrates strong intra-atomic 4f-5d exchange coupling. In addition, an ultrafast lattice contraction due to the release of magnetostriction leads to a transient shift of the magnetic satellite peak.

cond-mat.str-el↗

Ultrafast Laser-Induced Melting of Long-Range Magnetic Order in Multiferroic TbMnO3

We performed ultrafast time-resolved near-infrared pump, resonant soft X-ray diffraction probe measurements to investigate the coupling between the photoexcited electronic system and the spin cycloid magnetic order in multiferroic TbMnO3 at low temperatures. We observe melting of the long range antiferromagnetic order at low excitation fluences with a decay time constant of 22.3 +- 1.1 ps, which is much slower than the ~1 ps melting times previously observed in other systems. To explain the data we propose a simple model of the melting process where the pump laser pulse directly excites the electronic system, which then leads to an increase in the effective temperature of the spin system via a slower relaxation mechanism. Despite this apparent increase in the effective spin temperature, we do not observe changes in the wavevector q of the antiferromagnetic spin order that would typically correlate with an increase in temperature under equilibrium conditions. We suggest that this behavior results from the extremely low magnon group velocity that hinders a change in the spin-spiral wavevector on these time scales.

cond-mat.str-el↗

Coherent Acoustic Perturbation of Second-Harmonic-Generation in NiO

We investigate the structural and magnetic origins of the unusual ultrafast second-harmonicgeneration (SHG) response of femtosecond-laser-excited nickel oxide (NiO) previously attributed to oscillatory reorientation dynamics of the magnetic structure induced by d-d excitations. Using time-resolved x-ray diffraction from the (3/2 3/2 3/2) magnetic planes, we show that changes in the magnitude of the magnetic structure factor following ultrafast optical excitation are limited to $Δ / $ = 1.5% in the first 30 ps. An extended investigation of the ultrafast SHG response reveals a strong dependence on wavelength as well as characteristic echoes, both of which give evidence for an acoustic origin of the dynamics. We therefore propose an alternative mechanism for the SHG response based on perturbations of the nonlinear susceptibility via optically induced strain in a spatially confined medium. In this model, the two observed oscillation periods can be understood as the times required for an acoustic strain wave to traverse one coherence length of the SHG process in either the collinear or anti-collinear geometries.

cond-mat.str-el↗

Fermi surface of three-dimensional La1-xSrxMnO3 explored by soft-X-ray ARPES: Rhombohedral lattice distortion and its effect on magnetoresistance

Electronic structure of the three-dimensional colossal magnetoresistive perovskite La1-xSrxMnO3 has been established using soft-X-ray ARPES with its intrinsically sharp definition of three-dimensional electron momentum. The experimental results show much weaker polaronic coupling compared to the bilayer manganites and are consistent with the GGA+U band structure. The experimental Fermi surface unveils the canonical topology of alternating three-dimensional electron spheres and hole cubes, with their shadow contours manifesting the rhombohedral lattice distortion. This picture has been confirmed by one-step photoemission calculations including displacement of the apical oxygen atoms. The rhombohedral distortion is neutral to the Jahn-Teller effect and thus polaronic coupling, but affects the double-exchange electron hopping and thus the colossal magnetoresistance effect.

cond-mat.str-el↗

Ferro-type order of magneto-electric quadrupoles as an order-parameter for the pseudo-gap phase of a cuprate superconductor

Understanding the pseudo-gap phase from which a superconducting state emerges is a central problem in the physics of cuprates. The phase exists below a temperature T* for less than optimal doping of holes, and no clear jump in the specific heat or change in lattice symmetry is observed on crossing T*. Here we show that, two sets of intriguing experimental results in the literature concerning magnetic properties of underdoped YBCO are united in a single theory based on Cu quadrupole moments. The quadrupole is a product of spin and the electric dipole, so there is no magnetic dipole moment, and standard crystallography describes the magnetic motif. One experiment employed the Kerr effect and the second Bragg diffraction of polarized neutrons, and both are shown to imply an order-parameter for the pseudo-gap phase composed of magneto-electric quadrupoles at in-plane Cu sites in a ferro-type order. The successful interpretation of neutron diffraction data for YBCO yields the first experimental evidence that neutrons are deflected by magneto-electric multipoles. Predicted in 2014, our verification of the effect validates a new application for the experimental technique of choice in studies of magnetic motifs and excitations.

cond-mat.str-el↗

Ferro-type order of magneto-electric quadrupoles in the pseudo-gap phase of YBa2Cu3O6 + x unearthed by neutron diffraction

A theory that fully describes previously observed neutron Bragg spots indicative of magnetic order in the pseudo-gap phase of YBa2Cu3O6 + x is presented. Magnetic diffraction intensities, unveiled by polarization analysis, are explained by parity-violating magnetic (magneto-electric) quadrupoles at in-plane Cu sites arranged in a simple ferro-type motif. An absence of conventional spin and orbital angular momentum dipoles in the theory is compatible with the occurrence of superconductivity and strongly suggests, moreover, that magneto-electric quadrupoles are the primary order-parameter in the pseudo-gap phase.

cond-mat.str-el↗

Ultrafast structural dynamics of the Fe-pnictide parent compound BaFe2As2

Using femtosecond time-resolved x-ray diffraction we investigate the structural dynamics of the coherently excited A1g phonon mode in the Fe-pnictide parent compound BaFe2As2. The fluence dependent intensity oscillations of two specific Bragg reflections with distinctly different sensitivity to the pnictogen height in the compound allow us to quantify the coherent modifications of the Fe-As tetrahedra, indicating a transient increase of the Fe magnetic moments. By a comparison with time-resolved photoemission data we derive the electron-phonon deformation potential for this particular mode. The value of Delta mu/Delta z = -(1.0 - 1.5) eV/A is comparable with theoretical predictions and demonstrates the importance of this degree of freedom for the electron-phonon coupling in the Fe pnictides.

cond-mat.supr-con↗

Multiferroic properties of o-LuMnO$_3$ controlled by b-axis strain

Strain is a leading candidate for controlling magnetoelectric coupling in multiferroics. Here, we use x-ray diffraction to study the coupling between magnetic order and structural distortion in epitaxial films of the orthorhombic (o-) perovskite LuMnO$_3$. An antiferromagnetic spin canting in the E-type magnetic structure is shown to be related to the ferroelectrically induced structural distortion and to a change in the magnetic propagation vector. By comparing films of different orientations and thicknesses, these quantities are found to be controlled by b-axis strain. It is shown that compressive strain destabilizes the commensurate E-type structure and reduces its accompanying ferroelectric distortion.

cond-mat.str-el↗

Chiral properties of hematite (α-Fe2O3) inferred from resonant Bragg diffraction using circularly polarized x-rays

Chiral properties of the two phases - collinear motif (below Morin transition temperature, TM=250 K) and canted motif (above TM) - of magnetically ordered hematite (α-Fe2O3) have been identified in single crystal resonant x-ray Bragg diffraction, using circular polarized incident x-rays tuned near the iron K-edge. Magneto-electric multipoles, including an anapole, fully characterize the high-temperature canted phase, whereas the low-temperature collinear phase supports both parity-odd and parity-even multipoles that are time-odd. Orbital angular momentum accompanies the collinear motif, while it is conspicuously absent with the canted motif. Intensities have been successfully confronted with analytic expressions derived from an atomic model fully compliant with chemical and magnetic structures. Values of Fe atomic multipoles previously derived from independent experimental data, are shown to be completely trustworthy.

cond-mat.mtrl-sci↗

Dzyaloshinsky-Moriya driven helical-butterfly structure in Ba3NbFe3Si2O14

We have used soft x-ray magnetic diffraction at the Fe3+ L2,3 edges to examine to what extent the Dzyaloshinsky-Moriya interaction in Ba3NbFe3Si2O14 influences its low temperature magnetic structure. A modulated component of the moments along the c-axis is present, adding to the previously proposed helical magnetic configuration of co-planar moments in the a,b-plane. This leads to a helical-butterfly structure and suggests that both the multi-axial in-plane and the uniform out-of-plane Dzyaloshinsky-Moriya vectors are relevant. A non zero orbital magnetic signal is also observed at the oxygen K edge, which reflects the surprisingly strong hybridization between iron 3d and oxygen 2p states, given the nominal spherical symmetry of the Fe3+ half filled shell.

cond-mat.str-el↗

Identification of coherent lattice modulations coupled to charge and orbital order in a manganite

We apply grazing-incidence femtosecond x-ray diffraction to investigate the details of the atomic motion connected with a displacively excited coherent optical phonon. We concentrate on the low frequency phonon associated with the charge and orbital order in the mixed valence manganite La0.25Pr0.375Ca0.375MnO3 for T < 210 K. We measure the response of three superlattice reflections that feature different sensitivities to the motion of the unit cell constituents. The results support the assignment to a translational mode of the Mn4+ atoms together with the oxygen atoms connecting adjacent Mn4+ sites.

cond-mat.str-el↗

Phase competitions in epitaxial Pr$_{0.5}$Ca$_{0.5}$MnO$_3$/La$_{0.5}$Sr$_{0.5}$MnO$_3$ superlattices

We studied the charge-orbital ordering in the superlattice of charge-ordered insulating Pr$_{0.5}$Ca$_{0.5}$MnO$_3$ and ferromagnetic metallic La$_{0.5}$Sr$_{0.5}$MnO$_3$ by resonant soft x-ray diffraction. A temperature-dependent incommensurability is found in the orbital order. In addition, a large hysteresis is observed that is caused by phase competition between insulating charge ordered and metallic ferromagnetic states. No magnetic phase transitions are observed in contrast to bulk, confirming the unique character of the superlattice. The deviation from the commensurate orbital order can be directly related to the decrease of ordered-layer thickness that leads to a decoupling of the orbital-ordered planes along the c axis.

cond-mat.str-el↗

Imprinting magnetic information in manganites with X-rays

The effect of x-rays on an orbital and charge ordered epitaxial film of a Pr$_{0.5}$Ca$_{0.5}$MnO$_{3}$ is presented. As the film is exposed to x-rays, the antiferromagnetic response increases and concomitantly the conductivity of the film improve. These results are discussed in terms of a persistent x-ray induced doping, leading to a modification of the magnetic structure. This effect allows writing electronic and magnetic domains in the film and represents a novel way of manipulating magnetism.

cond-mat.str-el↗