Time-domain thermoreflectance (TDTR) characterization of FeRh throughout its first-order antiferromagnetic (AF) to ferromagnetic (FM) transition shows that the transient reflectance ΔR(t)/R strongly depends on the magnetic order of the sample. Using TDTR, which uses optical pulses to induce small temperature excursions, we have found that ΔR(t)/R of the AF phase exhibits a large negative response, while the response of the FM phase is positive. This magnetic phase sensitivity has allowed us to study the transient response of both the AF and FM phases to the pump-pulse excitation and the mixed phase of the material. These results are significant since the ultrafast properties of antiferromagnetic materials and mixed antiferromagnetic and ferromagnetic materials are difficult to detect using other conventional techniques. We have found that the AF phase exhibits a strong subpicosecond decaying signal not observed in the FM phase. The magnetic phase dependence of the sign of ΔR(t)/R is qualitatively explained using the results of ab initio density functional theory calculations. Using the two-temperature model, we found that the change in the thermalization time across the transition is caused by differences in both the electronic heat capacity and the electron-phonon coupling factor of the AF and FM phases. The electron-phonon coupling constant in the AF phase is also determined using the two-temperature model conducted using the ntmpy code package. For the FM phase, we provide boundaries for the magnitude of the electron-phonon coupling factor for the FM phase. These results indicate that TDTR can be used to study the transient properties of magnetic materials that are otherwise challenging to probe.

The advent of free electron lasers has opened the opportunity to explore interactions between extreme ultraviolet (EUV) photons and collective excitations in solids. While EUV transient grating spectroscopy, a noncollinear four-wave mixing technique, has already been applied to probe coherent phonons, the potential of EUV radiation for studying nanoscale spin waves has not been harnessed. Here we report EUV transient grating experiments with coherent magnons in Fe/Gd ferrimagnetic multilayers. Magnons with tens of nanometers wavelengths are excited by a pair of femtosecond EUV pulses and detected via diffraction of a probe pulse tuned to an absorption edge of Gd. The results unlock the potential of nonlinear EUV spectroscopy for studying magnons and provide a tool for exploring spin waves in a wave vector range not accessible by established inelastic scattering techniques.

Electromagnetic waves possessing orbital angular momentum (OAM) are powerful tools for applications in optical communications, quantum technologies, and optical tweezers. Recently, they have attracted growing interest since they can be harnessed to detect peculiar helical dichroic effects in chiral molecular media and in magnetic nanostructures. In this work, we perform single-shot per position ptychography on a nanostructured object at a seeded free-electron laser, using extreme ultraviolet OAM beams of different topological charge orders ℓ generated with spiral zone plates. By controlling ℓ, we demonstrate how the structural features of OAM beam profiles determine an improvement of about 30% in image resolution with respect to conventional Gaussian beam illumination. This result extends the capabilities of coherent diffraction imaging techniques, and paves the way for achieving time-resolved high-resolution (below 100 nm) microscopy on large area samples.

The ability to manipulate magnetic anisotropy is essential for magnetic sensing and storage tools. Surface carbon species offer cost-effective alternatives to metal-oxide and noble metal capping layers, inducing perpendicular magnetic anisotropy in ultrathin ferromagnetic films. Here, the different mechanisms by which the magnetism in a few-layer-thick Co thin film is modified upon adsorption of carbon monoxide (CO), dispersed carbon, and graphene are elucidated. Using X-ray microscopy with chemical and magnetic sensitivity, the in-plane to out-of-plane spin reorientation transition in cobalt is monitored during the accumulation of surface carbon up to the formation of graphene. Complementary magneto-optical measurements show weak perpendicular magnetic anisotropy (PMA) at room temperature for dispersed carbon on Co, while graphene-covered cobalt exhibits a significant out-of-plane coercive field. Density-functional theory (DFT) calculations show that going from CO/Co to C/Co and to graphene/Co, the magnetocrystalline and magnetostatic anisotropies combined promote out-of-plane magnetization. Anisotropy energies weakly depend on carbidic species coverage. Instead, the evolution of the carbon chemical state from carbidic to graphitic is accompanied by an exponential increase in the characteristic domain size, controlled by the magnetic anisotropy energy. Beyond providing a basic understanding of the carbon-ferromagnet interfaces, this study presents a sustainable approach to tailor magnetic anisotropy in ultrathin ferromagnetic films. Magnetic properties of Co ultrathin films are shown to undergo dramatic changes upon surface carbon accumulation. Chemical transformation from molecular carbon monoxide to surface carbide and to a graphene layer progressively enhances the perpendicular magnetic anisotropy of Co. Calculations reveal that magnetocrystalline and magnetostatic contributions play distinctly different roles for the different carbon species.image

The emergence of collective order in matter is among the most fundamental and intriguing phenomena in physics. In recent years, the dynamical control and creation of novel ordered states of matter not accessible in thermodynamic equilibrium is receiving much attention^1,2,3,4,5,6. The theoretical concept of dynamical multiferroicity has been introduced to describe the emergence of magnetization due to time-dependent electric polarization in non-ferromagnetic materials^7,8. In simple terms, the coherent rotating motion of the ions in a crystal induces a magnetic moment along the axis of rotation. Here we provide experimental evidence of room-temperature magnetization in the archetypal paraelectric perovskite SrTiO₃ due to this mechanism. We resonantly drive the infrared-active soft phonon mode with an intense circularly polarized terahertz electric field and detect the time-resolved magneto-optical Kerr effect. A simple model, which includes two coupled nonlinear oscillators whose forces and couplings are derived with ab initio calculations using self-consistent phonon theory at a finite temperature⁹, reproduces qualitatively our experimental observations. A quantitatively correct magnitude was obtained for the effect by also considering the phonon analogue of the reciprocal of the Einstein–de Haas effect, which is also called the Barnett effect, in which the total angular momentum from the phonon order is transferred to the electronic one. Our findings show a new path for the control of magnetism, for example, for ultrafast magnetic switches, by coherently controlling the lattice vibrations with light.

The THz Kerr effect measures the birefringence induced in an otherwise isotropic material by a strong THz pulse driving the Raman-active excitations of the systems. Here we provide experimental evidence of a sizable Kerr response in insulating SrTiO₃ due to infrared-active lattice vibrations. Such a signal, named the ionic Kerr effect, is associated with the simultaneous excitation of multiple phonons. Thanks to a theoretical modeling of the time, polarization, and temperature dependence of the birefrengence, we can disentangle the ionic Kerr effect from the off-resonant electronic excitations, providing an alternative tunable mechanism to modulate the refractive index on ultrashort timescales via infrared active phonons.

We describe the design of two types of metamaterials aimed at enhancing terahertz field pulses that can be used to control the magnetic state in condensed matter systems. The first structure is a so-called “dragonfly” antenna, able to realize a five-fold enhancement of the impinging terahertz magnetic field, while preserving its broadband features. For currently available state-of-the-art table top sources, this leads to peak magnetic fields exceeding 1 T. The second structure is an octopole antenna aimed at enhancing a circularly-polarized terahertz electric field, while preserving its polarization state. We obtain a five-fold enhancement of the electric field, hence expected to exceed the 1 MV/cm peak amplitude. Both our structures can be readily fabricated on top of virtually any material.

Artificial 2D van der Waals heterostructures with controllable vertical stacking and rotational orientation exhibit multifaceted electronic properties that are appealing for applications in fields ranging from optoelectronics to energy storage. Along with transition metal dichalcogenides and graphene, borophene has recently emerged as a promising building block for 2D devices due to its conductive nature as well as its exceptional mechanical and electronic properties. Here, it is demonstrated that the combination of the dissolution-segregation process and chemical vapor deposition allows for the synthesis of graphene/borophene heterostructures of the highest crystalline and chemical quality, in which graphene sits on top of the borophene layer with metallic character. The formation of laterally distinct micron-sized areas allows a comparative study of borophene, graphene, and the graphene–borophene heterostack in terms of their electronic properties and stability in a reactive environment. Whereas pristine borophene is particularly prone to oxidation, the graphene–borophene heterostack is chemically inert and enables the conservation of borophene's character even after exposure to air. This study opens up new perspectives for the scalable synthesis of graphene–borophene heterostacks with enhanced ability to preserve the metallic character and electronic properties of borophene. 

Energy-efficient spin-based technologies require new prospects for the realization of nanoscale logic devices that are able to operate at terahertz (THz) frequencies. For instance, in the field of magnonics, spin waves are proposed for data transport and processing. In this regard, magnonic concepts rely on generation of nanometer-wavelength spin waves, confined in a nanostructure. Here, we propose a layered metallic system, based on a ferromagnetic film sandwiched by heavy metals that allows a highly efficient coupling of millimeter wavelength THz light with nanometer-wavelength magnon modes. Using single-cycle broadband THz radiation, we are able to excite spin-wave modes with a frequency of up to 0.6 THz and a wavelength as short as 6 nm. Numerical simulations demonstrate that the coupling originates solely from interfacial spin-orbit torques. A possible origin of the enhanced damping of THz spin waves will be discussed.

Spin-based technologies can operate at terahertz frequencies but require manipulation techniques that work at ultrafast timescales to become practical. For instance, devices based on spin waves, also known as magnons, require efficient generation of high-energy exchange spin waves at nanometre wavelengths. To achieve this, a substantial coupling is needed between the magnon modes and an electro-magnetic stimulus such as a coherent terahertz field pulse. However, it has been difficult to excite non-uniform spin waves efficiently using terahertz light because of the large momentum mismatch between the submillimetre-wave radiation and the nanometre-sized spin waves. Here we improve the light–matter interaction by engineering thin films to exploit relativistic spin–orbit torques that are confined to the interfaces of heavy metal/ferromagnet heterostructures. We are able to excite spin-wave modes with frequencies of up to 0.6 THz and wavelengths as short as 6 nm using broadband terahertz radiation. Numerical simulations demonstrate that the coupling of terahertz light to exchange-dominated magnons originates solely from interfacial spin–orbit torques. Our results are of general applicability to other magnetic multilayered structures, and offer the prospect of nanoscale control of high-frequency signals.