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Interactions between the different degrees of freedom form the basis of many manifestations of intriguing physics in condensed matter. In this respect, quantifying the dynamics of normal modes that themselves arise from these interactions and how they interact with other excitations is of central importance. Of the different types of coupling that are often important, spin-lattice coupling is relevant to several sub-fields of condensed matter physics; examples include spintronics, high-TC superconductivity, and topological materials. While theories of materials where spin-lattice coupling is relevant can sometimes be used to infer the magnitude and character of this interaction, experimental approaches that can directly measure it are rare and incomplete. Here we use time-resolved X-ray diffraction to directly access the spin-lattice coupling by measuring both ultrafast atomic motion and the associated spin dynamics following the excitation of a coherent electromagnon by an intense THz pulse in a multiferroic hexaferrite. Comparing the dynamics of the two different components, one striking outcome is the different phase shifts relative to the driving field. This phase shift provides insight into the excitation process of such a coupled mode. This direct observation of combined lattice and magnetization dynamics paves the way to access the mode-selective spin-lattice coupling strength, which remains a missing fundamental parameter for ultrafast control of magnetism and is relevant to a wide variety of correlated electron physics., Comment: 4 figures

Optical-domain Transient Grating (TG) spectroscopy is a versatile background-free four-wave-mixing technique used to probe vibrational, magnetic and electronic degrees of freedom in the time domain. The newly developed coherent X-ray Free Electron Laser sources allow its extension to the X-ray regime. Xrays offer multiple advantages for TG: their large penetration depth allows probing the bulk properties of materials, their element-specificity can address core-excited states, and their short wavelengths create excitation gratings with unprecedented momentum transfer and spatial resolution. We demonstrate for the first time TG excitation in the hard X-ray range at 7.1 keV. In Bismuth Germanate (BGO), the nonresonant TG excitation generates coherent optical phonons detected as a function of time by diffraction of an optical probe pulse. This experiment demonstrates the ability to probe bulk properties of materials and paves the way for ultrafast coherent four-wave-mixing techniques using X-ray probes and involving nanoscale TG spatial periods., Comment: 11 pages, 4 figures

The interaction between phonons and high-energy excitations of electronic origin in cuprates and their role in the superconducting mechanisms is still controversial. Here we use coherent vibrational time-domain spectroscopy together with density functional and dynamical mean-field theory calculations to establish a direct link between the c-axis phonon modes and the in-plane electronic charge excitations in optimally doped YBCO. The non-equilibrium Raman tensor is measured by means of the broadband 'coherent-phonon' response in pump-probe experiments and is qualitatively described by our model using DFT in frozen phonon approximation plus single band DMFT to account for the electronic correlations. The major outcome of our experimental and theoretical study is to establish the link between out-of-plane copper ions displacements and the in-plane electronic correlations, and to estimate at few unit cells the correlation length of the associated phonon mode. The approach introduced here could help revealing the complex interplay between fluctuations of different nature and spatial correlation in several strongly-correlated materials., Comment: 13 pages, 6 figures, 24 panels

Atomically controlled crystal growth of thin films has established foundations of nanotechnology aimed at the development of advanced functional devices. Crystallization under non-equilibrium conditions allows engineering of new materials with their atomically-flat interfaces in the heterostructures exhibiting novel physical properties. From a fundamental point of view, knowledge of the electronic structures of thin films and their interfaces is indispensable to understand the origins of their functionality which further evolves into realistic device application. In view of extreme surface sensitivity of the conventional vacuum-ultraviolet (VUV) angle-resolved photoemission spectroscopy (ARPES), with a probing depth of several angstroms, experiments on thin films have to use sophisticated in-situ sample transfer systems to avoid surface contamination. In this Letter, we put forward a method to circumvent these difficulties using soft X-ray (SX) ARPES. A GaAs:Be thin film in our samples was protected by an amorphous As layer with an thickness of $\sim 1$ nm exceeding the probing depth of the VUV photoemission with photon energy $h\nu$ around 100 eV. The increase of the probing depth with increasing $h\nu$ towards the SX region has clearly exposed the bulk band dispersion without any surface treatment. Any contributions from potential interface states between the thin film and the amorphous capping layer has been below the detection limit. Our results demonstrate that SX-ARPES enables the observation of coherent three-dimensional band dispersion of buried heterostructure layers through an amorphous capping layer, breaking through the necessity of surface cleaning of thin film samples. Thereby, this opens new frontiers in diagnostics of authentic momentum-resolved electronic structure of protected thin-film heterostructures., Comment: 5 pages, 3 figures

Electronic structure of crystalline materials is their fundamental characteristic which is the basis of almost all their physical and chemical properties. Angle-resolved photoemission spectroscopy (ARPES) is the main experimental tool to study all electronic structure aspects with resolution in k-space. However, its application to three-dimensional (3D) materials suffers from a fundamental problem of ill-defined surface-perpendicular wavevector kz. Here, we achieve sharp definition of kz to enable precise navigation in 3D k space by pushing ARPES into the soft-X-ray photon energy range. Essential to break through the notorious problem of small photoexcitation cross-section was an advanced photon flux performance of our instrumentation. We explore the electronic structure of a transition metal dichalcogenide VSe2 which develops charge density waves (CDWs) possessing exotic 3D character. We experimentally identify nesting of its 3D Fermi surface (FS) as the precursor for these CDWs. Our study demonstrates an immense potential of soft-X-ray ARPES (SX-ARPES) to resolve various aspects of 3D electronic structure.

The spin texture of the metallic two-dimensional electron system (root3 x root3)-Au/Ge(111) is revealed by fully three-dimensional spin-resolved photoemission, as well as by density functional calculations. The large hexagonal Fermi surface, generated by the Au atoms, shows a significant splitting due to spin-orbit interactions. The planar components of the spin exhibit helical character, accompanied by a strong out-of-plane spin component with alternating signs along the six Fermi surface sections. Moreover, in-plane spin rotations towards a radial direction are observed close to the hexagon corners. Such a threefold-symmetric spin pattern is not described by the conventional Rashba model. Instead, it reveals an interplay with Dresselhaus-like spin-orbit effects as a result of the crystalline anisotropies., Comment: 5 pages, 4 figures, accepted at Physical Review Letters

Understanding the nature of electrical conductivity, superconductivity and magnetism between layers of oxides is of immense importance for the design of electronic devices employing oxide heterostructures. We demonstrate that resonant inelastic X-ray scattering can be applied to directly probe the carriers in oxide heterostructures. Our investigation on epitaxially grown LaAlO3/SrTiO3 superlattices unambiguously reveals the presence of both localized and delocalized Ti 3d carriers. These two types of carriers are caused by oxygen vacancies and electron transfer due to the polar discontinuity at the interface. This result allows explaining the reported discrepancy between theoretically calculated and experimentally measured carrier density values in LaAlO3/SrTiO3 heterostructures., Comment: 14 pages, 3 figures

Using a three-dimensional spin polarimeter we have gathered evidence for the interference of spin states in photoemission from the surface alloy Sb/Ag(111). This system features a small Rashba-type spin-splitting of a size comparable to the linewidth of the quasiparticles, thus causing an intrinsic overlap between states with orthogonal spinors. Besides a small spin polarization caused by the spin-splitting, we observe a large spin polarization component in the plane normal to the quantization axis provided by the Rashba effect. Strongly suggestive of coherent spin rotation, this effect is largely independent of the photon energy and photon polarization., Comment: 4 pages, 4 figures

Epitaxial graphene on SiC(0001) suffers from strong intrinsic n-type doping. We demonstrate that the excess negative charge can be fully compensated by non-covalently functionalizing graphene with the strong electron acceptor tetrafluorotetracyanoquinodimethane (F4-TCNQ). Charge neutrality can be reached in monolayer graphene as shown in electron dispersion spectra from angular resolved photoemission spectroscopy (ARPES). In bilayer graphene the band gap that originates from the SiC/graphene interface dipole increases with increasing F4-TCNQ deposition and, as a consequence of the molecular doping, the Fermi level is shifted into the band gap. The reduction of the charge carrier density upon molecular deposition is quantified using electronic Fermi surfaces and Raman spectroscopy. The structural and electronic characteristics of the graphene/F4-TCNQ charge transfer complex are investigated by X-ray photoelectron spectroscopy (XPS) and ultraviolet photoelectron spectroscopy (UPS). The doping effect on graphene is preserved in air and is temperature resistant up to 200\degree C. Furthermore, graphene non-covalent functionalization with F4-TCNQ can be implemented not only via evaporation in ultra-high vacuum but also by wet chemistry.

The Fermi and Rashba energies of surface states in the Bi_xPb_{1-x}/Ag(111) alloy can be tuned simultaneously by changing the composition parameter x. We report on unconventional Fermi surface spin textures observed by spin and angle-resolved photoemission spectroscopy {that are correlated with a topological transition of the Fermi surface occurring at x=0.5. We show that the surface states remain fully spin polarized upon alloying and that the spin polarization vectors are approximately tangential to the constant energy contours. We discuss the implications of the topological transition for the transport of spin., Comment: 5 pages, 5 figures

A Rashba type spin-orbit splitting is found for quantum well states formed in ultrathin Pb films on Si(111). The resulting momentum splitting is comparable to what is found for semiconductor heterostructures. The splitting shows no coverage dependency and the sign of the spin polarization is reversed compared to Rashba splitting in the Au(111) surface state. We explain our results by competing effects at the two boundaries of the Pb layer.

The concept of vectorial spin analysis in spin and angle resolved photoemission is illustrated in this report. Two prototypical systems, Bi/Ag(111)(sqrt3 x sqrt3)R30 and Pb/Ag(111)(sqrt3 x sqrt3)R30, which show a large Rashba type spin-orbit splitting, were investigated by means of spin and angle resolved photoemission. The spin polarization vectors of individual bands are determined by a two-step fitting routine. First, the measured intensities are fitted with an appropriate number of suitable peaks to quantify the contributions of the individual bands, then the measured spin polarization curves are fitted by varying for each band the polarization direction and its magnitude. We confirm that the surface states experience a large spin splitting. Moreover, we find that all surface state bands are 100 percent spin polarized, and that for some states spin polarization vectors rotate out of the surface plane., Comment: 9 pages, 2 tables, 8 figures