The fluctuation-dissipation measurement instrument at the Linac Coherent Light Source.

The development of new modes at x-ray free electron lasers has inspired novel methods for studying fluctuations at different energies and timescales. For closely spaced x-ray pulses that can be varied on ultrafast time scales, we have constructed a pair of advanced instruments to conduct studies targeting quantum materials. We first describe a prototype instrument built to test the proof-of-principle of resonant magnetic scattering using ultrafast pulse pairs. This is followed by a description of a new endstation, the so-called fluctuation-dissipation measurement instrument, which was used to carry out studies with a fast area detector. In addition, we describe various types of diagnostics for single-shot contrast measurements, which can be used to normalize data on a pulse-by-pulse basis and calibrate pulse amplitude ratios, both of which are important for the study of fluctuations in materials. Furthermore, we present some new results using the instrument that demonstrates access to higher momentum resolution.

Ultrafast kinetics of the antiferromagnetic-ferromagnetic phase transition in FeRh.

Understanding how fast short-range interactions build up long-range order is one of the most intriguing topics in condensed matter physics. FeRh is a test specimen for studying this problem in magnetism, where the microscopic spin-spin exchange interaction is ultimately responsible for either ferro- or antiferromagnetic macroscopic order. Femtosecond laser excitation can induce ferromagnetism in antiferromagnetic FeRh, but the mechanism and dynamics of this transition are topics of intense debates. Employing double-pump THz emission spectroscopy has enabled us to dramatically increase the temporal detection window of THz emission probes of transient states without sacrificing any loss of resolution or sensitivity. It allows us to study the kinetics of emergent ferromagnetism from the femtosecond up to the nanosecond timescales in FeRh/Pt bilayers. Our results strongly suggest a latency period between the initial pump-excitation and the emission of THz radiation by ferromagnetic nuclei.

Femtosecond control of phonon dynamics near a magnetic order critical point.

The spin-phonon interaction in spin density wave (SDW) systems often determines the free energy landscape that drives the evolution of the system. When a passing energy flux, such as photoexcitation, drives a crystalline system far from equilibrium, the resulting lattice displacement generates transient vibrational states. Manipulating intermediate vibrational states in the vicinity of the critical point, where the SDW order parameter changes dramatically, would then allow dynamical control over functional properties. Here we combine double photoexcitation with an X-ray free-electron laser (XFEL) probe to control and detect the lifetime and magnitude of the intermediate vibrational state near the critical point of the SDW in chromium. We apply Landau theory to identify the mechanism of control as a repeated partial quench and sub picosecond recovery of the SDW. Our results showcase the capabilities to influence and monitor quantum states by combining multiple optical photoexcitations with an XFEL probe. They open new avenues for manipulating and researching the behaviour of photoexcited states in charge and spin order systems near the critical point.

Scaling of domain cascades in stripe and skyrmion phases.

The origin of deterministic macroscopic properties often lies in microscopic stochastic motion. Magnetic fluctuations that manifest as domain avalanches and chaotic magnetization jumps exemplify such stochastic motion and have been studied in great detail. Here we report Fourier space studies of avalanches in a system exhibiting competing magnetic stripe and skyrmion phase using a soft X-ray speckle metrology technique. We demonstrate the existence of phase boundaries and underlying critical points in the stripe and skyrmion phases. We found that distinct scaling and universality classes are associated with these domain topologies. The magnitude and frequency of abrupt magnetic domain jumps observed in the stripe phase are dramatically reduced in the skyrmion phase. Our results provide an incisive way to probe and understand phase stability in systems exhibiting complex spin topologies.

Publisher Correction: Scaling of domain cascades in stripe and skyrmion phases.

The original version of this Article contained an error in Fig. 4d, in which the label of the region to the left of the white dashed lines incorrectly read 'Order stripes'. The correct version states 'Disorder stripes'. This has been corrected in both the PDF and HTML versions of the Article.

Publisher Correction: Beyond a phenomenological description of magnetostriction.

"The technical support from SLAC Accelerator Directorate, Technology Innovation Directorate, LCLS laser division and Test Facility Division is gratefully acknowledged. We thank S.P. Weathersby, R.K. Jobe, D. McCormick, A. Mitra, S. Carron and J. Corbett for their invaluable help and technical assistance. Research at SLAC was supported through the SIMES Institute which like the LCLS and SSRL user facilities is funded by the Office of Basic Energy Sciences of the U.S. Department of Energy under Contract No. DE-AC02-76SF00515. The UED work was performed at SLAC MeV-UED, which is supported in part by the DOE BES SUF Division Accelerator & Detector R&D program, the LCLS Facility, and SLAC under contract Nos. DE-AC02-05-CH11231 and DE-AC02-76SF00515. Use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515."and"Work at BNL was supported by DOE BES Materials Science and Engineering Division under Contract No: DE-AC02-98CH10886. J.C. would like to acknowledge the support from National Science Foundation Grant No. 1207252. E.E.F. would like to acknowledge support from the U.S. Department of Energy (DOE), Office of Basic Energy Sciences (BES) under Award No. DE-SC0003678."This has been corrected in both the PDF and HTML versions of the Article.

Beyond a phenomenological description of magnetostriction.

Magnetostriction, the strain induced by a change in magnetization, is a universal effect in magnetic materials. Owing to the difficulty in unraveling its microscopic origin, it has been largely treated phenomenologically. Here, we show how the source of magnetostriction-the underlying magnetoelastic stress-can be separated in the time domain, opening the door for an atomistic understanding. X-ray and electron diffraction are used to separate the sub-picosecond spin and lattice responses of FePt nanoparticles. Following excitation with a 50-fs laser pulse, time-resolved X-ray diffraction demonstrates that magnetic order is lost within the nanoparticles with a time constant of 146 fs. Ultrafast electron diffraction reveals that this demagnetization is followed by an anisotropic, three-dimensional lattice motion. Analysis of the size, speed, and symmetry of the lattice motion, together with ab initio calculations accounting for the stresses due to electrons and phonons, allow us to reveal the magnetoelastic stress generated by demagnetization.

Nanosecond X-Ray Photon Correlation Spectroscopy on Magnetic Skyrmions.

We report an x-ray photon correlation spectroscopy method that exploits the recent development of the two-pulse mode at the Linac Coherent Light Source. By using coherent resonant x-ray magnetic scattering, we studied spontaneous fluctuations on nanosecond time scales in thin films of multilayered Fe/Gd that exhibit ordered stripe and Skyrmion lattice phases. The correlation time of the fluctuations was found to differ between the Skyrmion phase and near the stripe-Skyrmion boundary. This technique will enable a significant new area of research on the study of equilibrium fluctuations in condensed matter.

Luminescent hyperbolic metasurfaces.

When engineered on scales much smaller than the operating wavelength, metal-semiconductor nanostructures exhibit properties unobtainable in nature. Namely, a uniaxial optical metamaterial described by a hyperbolic dispersion relation can simultaneously behave as a reflective metal and an absorptive or emissive semiconductor for electromagnetic waves with orthogonal linear polarization states. Using an unconventional multilayer architecture, we demonstrate luminescent hyperbolic metasurfaces, wherein distributed semiconducting quantum wells display extreme absorption and emission polarization anisotropy. Through normally incident micro-photoluminescence measurements, we observe absorption anisotropies greater than a factor of 10 and degree-of-linear polarization of emission >0.9. We observe the modification of emission spectra and, by incorporating wavelength-scale gratings, show a controlled reduction of polarization anisotropy. We verify hyperbolic dispersion with numerical simulations that model the metasurface as a composite nanoscale structure and according to the effective medium approximation. Finally, we experimentally demonstrate >350% emission intensity enhancement relative to the bare semiconducting quantum wells.

Colossal magnetic phase transition asymmetry in mesoscale FeRh stripes.

Coupled order parameters in phase-transition materials can be controlled using various driving forces such as temperature, magnetic and electric field, strain, spin-polarized currents and optical pulses. Tuning the material properties to achieve efficient transitions would enable fast and low-power electronic devices. Here we show that the first-order metamagnetic phase transition in FeRh films becomes strongly asymmetric in mesoscale structures. In patterned FeRh stripes we observed pronounced supercooling and an avalanche-like abrupt transition from the ferromagnetic to the antiferromagnetic phase, while the reverse transition remains nearly continuous over a broad temperature range. Although modest asymmetry signatures have been found in FeRh films, the effect is dramatically enhanced at the mesoscale. The activation volume of the antiferromagnetic phase is more than two orders of magnitude larger than typical magnetic heterogeneities observed in films. The collective behaviour upon cooling results from the role of long-range ferromagnetic exchange correlations that become important at the mesoscale and should be a general property of first-order metamagnetic phase transitions.

Photoinduced Enhancement of the Charge Density Wave Amplitude.

Symmetry breaking and the emergence of order is one of the most fascinating phenomena in condensed matter physics. It leads to a plethora of intriguing ground states found in antiferromagnets, Mott insulators, superconductors, and density-wave systems. Exploiting states of matter far from equilibrium can provide even more striking routes to symmetry-lowered, ordered states. Here, we demonstrate for the case of elemental chromium that moderate ultrafast photoexcitation can transiently enhance the charge-density-wave (CDW) amplitude by up to 30% above its equilibrium value, while strong excitations lead to an oscillating, large-amplitude CDW state that persists above the equilibrium transition temperature. Both effects result from dynamic electron-phonon interactions, providing an efficient mechanism to selectively transform a broad excitation of the electronic order into a well-defined, long-lived coherent lattice vibration. This mechanism may be exploited to transiently enhance order parameters in other systems with coupled degrees of freedom.

All-optical control of ferromagnetic thin films and nanostructures.

The interplay of light and magnetism allowed light to be used as a probe of magnetic materials. Now the focus has shifted to use polarized light to alter or manipulate magnetism. Here, we demonstrate optical control of ferromagnetic materials ranging from magnetic thin films to multilayers and even granular films being explored for ultra-high-density magnetic recording. Our finding shows that optical control of magnetic materials is a much more general phenomenon than previously assumed and may have a major impact on data memory and storage industries through the integration of optical control of ferromagnetic bits.

Investigating the role of superdiffusive currents in laser induced demagnetization of ferromagnets with nanoscale magnetic domains.

Understanding the loss of magnetic order and the microscopic mechanisms involved in laser induced magnetization dynamics is one of the most challenging topics in today's magnetism research. While scattering between spins, phonons, magnons and electrons have been proposed as sources for dissipation of spin angular momentum, ultrafast spin dependent transport of hot electrons has been pointed out as a potential candidate to explain ultrafast demagnetization without resorting to any spin dissipation channel. Here we use time resolved magneto-optical Kerr measurements to extract the influence of spin dependent transport on the demagnetization dynamics taking place in magnetic samples with alternating domains with opposite magnetization directions. We unambiguously show that whatever the sample magnetic configuration, the demagnetization takes place during the same time, demonstrating that hot electrons spin dependent transfer between neighboring domains does not alter the ultrafast magnetization dynamics in our systems with perpendicular anisotropy and 140 nm domain sizes.

Engineered materials for all-optical helicity-dependent magnetic switching.

The possibility of manipulating magnetic systems without applied magnetic fields have attracted growing attention over the past fifteen years. The low-power manipulation of the magnetization, preferably at ultrashort timescales, has become a fundamental challenge with implications for future magnetic information memory and storage technologies. Here we explore the optical manipulation of the magnetization in engineered magnetic materials. We demonstrate that all-optical helicity-dependent switching (AO-HDS) can be observed not only in selected rare earth-transition metal (RE-TM) alloy films but also in a much broader variety of materials, including RE-TM alloys, multilayers and heterostructures. We further show that RE-free Co-Ir-based synthetic ferrimagnetic heterostructures designed to mimic the magnetic properties of RE-TM alloys also exhibit AO-HDS. These results challenge present theories of AO-HDS and provide a pathway to engineering materials for future applications based on all-optical control of magnetic order.

Dynamic switching of the spin circulation in tapered magnetic nanodisks.

Magnetic vortices are characterized by the sense of in-plane magnetization circulation and by the polarity of the vortex core. With each having two possible states, there are four possible stable magnetization configurations that can be utilized for a multibit memory cell. Dynamic control of vortex core polarity has been demonstrated using both alternating and pulsed magnetic fields and currents. Here, we show controlled dynamic switching of spin circulation in vortices using nanosecond field pulses by imaging the process with full-field soft X-ray transmission microscopy. The dynamic reversal process is controlled by far-from-equilibrium gyrotropic precession of the vortex core, and the reversal is achieved at significantly reduced field amplitudes when compared with static switching. We further show that both the field pulse amplitude and duration required for efficient circulation reversal can be controlled by appropriate selection of the disk geometry.

Fe spin reorientation across the metamagnetic transition in strained FeRh thin films.

A spin reorientation accompanying the temperature-induced antiferromagnetic (AFM) to ferromagnetic (FM) phase transition is reported in strained epitaxial FeRh thin films. (57)Fe conversion electron Mössbauer spectrometry showed that the Fe moments have different orientations in FeRh grown on thick single-crystalline MgO and in FeRh grown on ion-beam-assist-deposited (IBAD) MgO. It was also observed, in both samples, that the Fe moments switch orientations at the AFM to FM phase transition. Perpendicular anisotropy was evidenced in the AFM phase of the film grown on IBAD MgO and in the FM phase of that grown on regular MgO. Density-functional theory calculations enabled this spin-reorientation transition to be accurately reproduced for both FeRh films across the AFM-FM phase transition and show that these results are due to differences in strain.

Electronic structure changes across the metamagnetic transition in FeRh via hard X-ray photoemission.

Stoichiometric FeRh undergoes a temperature-induced antiferromagnetic (AFM) to ferromagnetic (FM) transition at ~350 K. In this Letter, changes in the electronic structure accompanying this transition are investigated in epitaxial FeRh thin films via bulk-sensitive valence-band and core-level hard x-ray photoelectron spectroscopy with a photon energy of 5.95 keV. Clear differences between the AFM and FM states are observed across the entire valence-band spectrum and these are well reproduced using density-functional theory. Changes in the 2p core levels of Fe are also observed and interpreted using Anderson impurity model calculations. These results indicate that significant electronic structure changes over the entire valence-band region are involved in this AFM-FM transition.

Structural and magnetic dynamics of a laser induced phase transition in FeRh.

We use time-resolved x-ray diffraction and magneto-optical Kerr effect to study the laser-induced antiferromagnetic to ferromagnetic phase transition in FeRh. The structural response is given by the nucleation of independent ferromagnetic domains (τ(1)~30 ps). This is significantly faster than the magnetic response (τ(2)~60 ps) given by the subsequent domain realignment. X-ray diffraction shows that the two phases coexist on short time scales and that the phase transition is limited by the speed of sound. A nucleation model describing both the structural and magnetic dynamics is presented.

Thermodynamic measurements of Fe-Rh alloys.

FeRh undergoes an unusual antiferromagnetic-to-ferromagnetic (AFM-FM) transition just above room temperature (T(AFM>FM)) that can be tuned or even completely suppressed with small changes in composition. The underlying temperature-dependent entropy difference between the competing AFM and FM states that drives this transition is measured by specific heat as a function of temperature from 2 to 380 K on two nearly equiatomic epitaxial Fe-Rh films, one with a ferromagnetic ground state (Fe-rich) and the other with an antiferromagnetic ground state (Rh-rich). The FM state shows an excess heat capacity near 100 K associated with magnetic excitations that are not present in the AFM state. The integrated entropy and enthalpy differences between the two alloys up to T(AFM>FM) agree with the previously measured entropy of the transition (ΔS = 17 ± 3 J/kg/K) and yield a T=0 energy difference of 3.4 J/g, consistent with literature calculations and experimental data; this agreement supports the use of the Fe-rich FM sample as a proxy for the (unstable) FM state of the AFM Rh-rich sample. From the low-temperature specific heat, along with sound velocity and photoemission measurements, the lattice contribution to the difference (ΔS(latt) = -33 ± 9 J/kg/K) and electronic contribution (ΔS(el) = 8 ± 1 J/kg/K) to the difference in entropy are calculated, from which the excess heat capacity in the FM phase and the resulting entropy difference are shown to be dominated by magnetic fluctuations (ΔS(mag) = 43 ± 9 J/kg/K). The excess magnetic heat capacity is dominated by the magnetic heat capacity of the FM phase, which can be fit to a Schottky-like anomaly with an energy splitting of 16 ± 1 meV and a multiplicity of 1 per unit cell.

Calorimetry of epitaxial thin films.

Thin film growth allows for the manipulation of material on the nanoscale, making possible the creation of metastable phases not seen in the bulk. Heat capacity provides a direct way of measuring thermodynamic properties of these new materials, but traditional bulk calorimetric techniques are inappropriate for such a small amount of material. Microcalorimetry and nanocalorimetry techniques exist for the measurements of thin films but rely on an amorphous membrane platform, limiting the types of films which can be measured. In the current work, ion-beam-assisted deposition is used to provide a biaxially oriented MgO template on a suspended membrane microcalorimeter in order to measure the specific heat of epitaxial thin films. Synchrotron x-ray diffraction showed the biaxial order of the MgO template. X-ray diffraction was also used to prove the high quality of epitaxy of a film grown onto this MgO template. The contribution of the MgO layer to the total heat capacity was measured to be just 6.5% of the total addenda contribution. The heat capacity of a Fe(.49)Rh(.51) film grown epitaxially onto the device was measured, comparing favorably to literature data on bulk crystals. This shows the viability of the MgO∕SiN(x)-membrane-based microcalorimeter as a way of measuring the thermodynamic properties of epitaxial thin films.