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We report a soft x-ray resonant magnetic scattering study of the spin configuration in multiferroic thin films of ${\mathrm{Co}}_{0.975}{\mathrm{Ge}}_{0.025}{\mathrm{Cr}}_{2}{\mathrm{O}}_{4}$ (Ge-CCO) and ${\mathrm{CoCr}}_{2}{\mathrm{O}}_{4}$ (CCO) under low and high magnetic fields from 0.2 to 6.5 T. A characterization of Ge-CCO at a low magnetic field was performed, and the results were compared with those of pure CCO. The ferrimagnetic phase transition temperature ${T}_{C}\ensuremath{\approx}95\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ and the multiferroic transition temperature ${T}_{S}\ensuremath{\approx}27\phantom{\rule{0.28em}{0ex}}\mathrm{K}$ in Ge-CCO are comparable with those observed in CCO. In Ge-CCO, the ordering wave vector ($qq0$) observed below ${T}_{S}$ is slightly larger compared with that of CCO, and unlike CCO, the diffraction intensity consists of two contributions that show a dissimilar x-ray polarization dependence. In Ge-CCO, the coercive field observed at low temperatures was larger than the one reported for CCO. In both compounds, an unexpected reversal of the spiral helicity, and therefore the electric polarization, was observed on simply magnetic field cooling. In addition, we find a change in the helicity as a function of momentum transfer in the magnetic diffraction peak of Ge-CCO, indicative of the presence of multiple magnetic spirals.

The authors find that the structural distortion and the underlying electronic structure of the charge density wave in TiSe${}_{2}$ show different energetics at ultrafast timescales.

Orthorhombic $\mathrm{HoMn}{\mathrm{O}}_{3}$ is a multiferroic in which Mn antiferromagnetic order induces ferroelectricity. A second transition occurs within the multiferroic phase, in which a strong enhancement of the ferroelectric polarization occurs concomitantly to antiferromagnetic ordering of Ho $4f$ magnetic moments. Using the element selectivity of resonant x-ray diffraction, we study the magnetic order of the Mn $3d$ and Ho $4f$ moments. We explicitly show that the Mn magnetic order is affected by the Ho $4f$ magnetic ordering transition. Based on the azimuthal dependence of the $(0\phantom{\rule{0.16em}{0ex}}q\phantom{\rule{0.16em}{0ex}}0)$ and $(0\phantom{\rule{0.16em}{0ex}}1\ensuremath{-}q\phantom{\rule{0.16em}{0ex}}0)$ magnetic reflections, we suggest that the Ho $4f$ order resembles an $ac$ cycloid. Using nonresonant diffraction, we show that the magnetically induced polar lattice distortion is unaffected by the Ho ordering, suggesting a mechanism through which the Ho order affects ferroelectric polarization without affecting the lattice in the same manner as the Mn order.

ACS applied materials & interfaces 12(7), 8780 - 8787 (2020). doi:10.1021/acsami.9b15034, Hybrid semiconductor���ferromagnetic insulator heterostructures are interesting due to their tunable electronic transport, self-sustained stray field, and local proximitized magnetic exchange. In this work, we present lattice-matched hybrid epitaxy of semiconductor���ferromagnetic insulator InAs/EuS heterostructures and analyze the atomic-scale structure and their electronic and magnetic characteristics. The Fermi level at the InAs/EuS interface is found to be close to the InAs conduction band and in the band gap of EuS, thus preserving the semiconducting properties. Both neutron and X-ray reflectivity measurements show that the overall ferromagnetic component is mainly localized in the EuS thin film with a suppression of the Eu moment in the EuS layer nearest the InAs and magnetic moments outside the detection limits on the pure InAs side. This work presents a step toward realizing defect-free semiconductor���ferromagnetic insulator epitaxial hybrids for spin-lifted quantum and spintronic applications without external magnetic fields., Published by Soc., Washington, DC

We use resonant and non-resonant X-ray diffraction measurements in combination with first-principles electronic structure calculations and Monte Carlo simulations to study the relationship between crystal structure and multiferroic orders in the orthorhombic perovskite manganites, o-$R$MnO$_3$ ($R$ is a rare-earth cation or Y). In particular, we focus on how the internal lattice parameters (Mn-O bond lengths and Mn-O-Mn bond angles) evolve under chemical pressure and epitaxial strain, and the effect of these structural variations on the microscopic exchange interactions and long-range magnetic order. We show that chemical pressure and epitaxial strain are accommodated differently by the crystal lattice of o-$R$MnO$_3$, which is key for understanding the difference in magnetic properties between bulk samples and strained films. Finally, we discuss the effects of these differences in the magnetism on the electric polarization in o-$R$MnO$_3$., Comment: 16 pages, 10 figures

X-ray magnetic circular dichroism (XMCD) and x-ray magnetic linear dichroism (XMLD) have been used to investigate the Fe magnetic response during the spin-reorientation transition (SRT) in $\mathrm{TmFe}{\mathrm{O}}_{3}$. Comparing the Fe XMLD results with neutron-diffraction and magnetization measurements on the same sample indicates that the SRT has an enhanced temperature range in the near surface region of approximately 82 to 120 K compared to approximately 82 to 92 K in bulk. This view is supported by complementary resonant soft x-ray-diffraction experiments at the Tm ${M}_{5}$ edge. These measurements find an induced magnetic moment on the Tm sites, which is well described by a dipolar mean-field model originating from the Fe moments. Even though such a model can describe the $4f$ response in the experiments, it is insufficient to describe the SRT even when considering a change in the $4f$ anisotropy. Moreover, the results of the Fe XMCD show a different temperature evolution through the SRT, the interpretation of which is hampered by additional spectral shape changes of the XCMD signal.

Using resonant soft x-ray techniques we follow the magnetic behavior of a strained epitaxial film of $\mathrm{CoC}{\mathrm{r}}_{2}{\mathrm{O}}_{4}$, 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 (RXD) 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 ${T}_{C}\ensuremath{\approx}90\phantom{\rule{4pt}{0ex}}\mathrm{K}$, 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 $\mathrm{C}{\mathrm{o}}^{2+}$ orbital moment (${m}_{L}$) is found, which can explain this hardening. The RXD signal of the (q q 0) reflection appears below ${T}_{S}$, 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.

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 ${\mathrm{Ba}}_{3}{\mathrm{TaFe}}_{3}{\mathrm{Si}}_{2}{\mathrm{O}}_{14}$ at the Fe ${L}_{2,3}$ and oxygen $K$ edges. Below ${T}_{N}$ ($\ensuremath{\approx}27K$) we observe the satellite reflections $(0,0,\ensuremath{\tau}), (0,0,2\ensuremath{\tau}), (0,0,3\ensuremath{\tau})$, and $(0,0,1\ensuremath{-}3\ensuremath{\tau})$ where $\ensuremath{\tau}\ensuremath{\approx}0.140\ifmmode\pm\else\textpm\fi{}0.001$. 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 ($\stackrel{\ifmmode \hat{}\else \^{}\fi{}}{\mathbf{c}}$ axis) magnetic dipole while the $(0,0,2\ensuremath{\tau})$ originates from the electron density distortions accompanying magnetic order. We observe dissimilar energy dependencies 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.

We investigate the demagnetization dynamics of the cycloidal and sinusoidal phases of multiferroic TbMnO3 by means of time-resolved resonant soft x-ray diffraction following excitation by an optical pump. The use of orthogonal linear x-ray polarizations provides information on the contribution from the different magnetic moment directions, which can be interpreted as signatures from multiferroic cycloidal spin order and sinusoidal spin order. Tracking these signatures in the time domain enables us to identify the transient magnetic phase created by intense photoexcitation of the electrons and subsequent heating of the spin system on a picosecond time scale. The transient phase is shown to exhibit mostly spin density wave character, as in the adiabatic case, while nevertheless retaining the wave vector of the cycloidal long-range order. Two different pump photon energies, 1.55 and 3.1 eV, lead to population of the conduction band predominantly via intersite d-d or intrasite p-d transitions, respectively. We find that the nature of the optical excitation does not play an important role in determining the dynamics of magnetic order melting. Further, we observe that the orbital reconstruction, which is induced by the spin ordering, disappears on a time scale comparable to that of the cycloidal order, attesting to a direct coupling between magnetic order and orbital reconstruction. Our observations are discussed in the context of recent theoretical models of demagnetization dynamics in strongly correlated systems, revealing the potential of this type of measurement as a benchmark for such theoretical studies.

We investigated the crystal structure and lattice excitations of the ternary intermetallic stannide Ca3Ir4Sn13 using neutron and x-ray scattering techniques. For T > T* ~ 38 K the x-ray diffraction data can be satisfactorily refined using the space group Pm-3n. Below T* the crystal structure is modulated with a propagation vector of q = (1/2, 1/2, 0). This may arise from a merohedral twinning in which three tetragonal domains overlap to mimic a higher symmetry, or from a doubling of the cubic unit cell. Neutron diffraction and neutron spectroscopy results show that the structural transition at T* is of a second-order, and that it is well described by mean-field theory. Inelastic neutron scattering data point towards a displacive structural transition at T* arising from the softening of a low-energy phonon mode with an energy gap of Delta(120 K) = 1.05 meV. Using density functional theory the soft phonon mode is identified as a 'breathing' mode of the Sn12 icosahedra and is consistent with the thermal ellipsoids of the Sn2 atoms found by single crystal diffraction data.

Using the small angle neutron scattering (SANS) technique we investigated the vortex lattice (VL) in the mixed state of the stannide superconductor Yb$_{3}$Rh$_{4}$Sn$_{13}$. We find a single domain VL of slightly distorted hexagonal geometry for field strengths between 350 and 18500 G and temperatures between T = 0.05 and T = 6.5 K. We observe a clear in-plane rotation of the VL for different magnetic field directions relative to the crystallographic axes. We also find that the hexagonal symmetry of the VL is energetically favorable in Yb$_{3}$Rh$_{4}$Sn$_{13}$ for external fields oriented along axes of different symmetries: twofold [110], threefold [111] and fourfold [100]. The observed behavior is different from other conventional and unconventional superconductors. The superconducting state is characterized by an isotropic gapped order parameter with an amplitude of $\Delta(0)$ = 1.57 $\pm$ 0.05 meV. At the lowest temperatures the field dependence of the magnetic form factor in our material reveals a London penetration depth of $\lambda_{L}$ = 2508 $\pm$ 17 $\AA$ and a Ginzburg coherence length of $\xi$ = 100 $\pm$ 1.3 $\AA$, i.e., it is a strongly type-II superconductor, $\kappa$ = $\lambda_{L}/\xi$ = 25.

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., submitted to Applied Physics Letters

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 wave vector 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 wave vector on these time scales. DOI: 10.1103/PhysRevB.92.184429

The correlation between electronic and crystal structures of 1T-TiSe2 in the charge density wave (CDW) state is studied by x-ray diffraction. Three families of reflections are used to probe atomic displacements and the orbital asymmetry in Se. Two distinct onset temperatures are found, TCDW and a lower T* indicative for an onset of Se out-of-plane atomic displacements. T* coincides with a DC resistivity maximum and the onset of the proposed gyrotropic electronic structure. However, no indication for chirality is found. The relation between the atomic displacements and the transport properties is discussed in terms of Ti 3d and Se 4p states that only weakly couple to the CDW order., Comment: 16 pages, 4 figures + 13 pages supplementary info