The 2024 magnonics roadmap.

Magnonicsis a research field that has gained an increasing interest in both the fundamental and applied sciences in recent years. This field aims to explore and functionalize collective spin excitations in magnetically ordered materials for modern information technologies, sensing applications and advanced computational schemes. Spin waves, also known as magnons, carry spin angular momenta that allow for the transmission, storage and processing of information without moving charges. In integrated circuits, magnons enable on-chip data processing at ultrahigh frequencies without the Joule heating, which currently limits clock frequencies in conventional data processors to a few GHz. Recent developments in the field indicate that functional magnonic building blocks for in-memory computation, neural networks and Ising machines are within reach. At the same time, the miniaturization of magnonic circuits advances continuously as the synergy of materials science, electrical engineering and nanotechnology allows for novel on-chip excitation and detection schemes. Such circuits can already enable magnon wavelengths of 50 nm at microwave frequencies in a 5G frequency band. Research into non-charge-based technologies is urgently needed in view of the rapid growth of machine learning and artificial intelligence applications, which consume substantial energy when implemented on conventional data processing units. In its first part, the 2024 Magnonics Roadmap provides an update on the recent developments and achievements in the field of nano-magnonics while defining its future avenues and challenges. In its second part, the Roadmap addresses the rapidly growing research endeavors on hybrid structures and magnonics-enabled quantum engineering. We anticipate that these directions will continue to attract researchers to the field and, in addition to showcasing intriguing science, will enable unprecedented functionalities that enhance the efficiency of alternative information technologies and computational schemes.

Terahertz wave rectification in a ferroelectric triglycine sulfate single crystal.

The effect of optical rectification (OR) in the terahertz range (THz rectification, TR) is experimentally demonstrated. The effect consists of generating a DC voltage on the faces of a ferroelectric triglycine sulfate (TGS) single crystal under the action of pulsed radiation with a frequency of 1.57 and 1.96 THz and an electric field strength per pulse of 1.3 and 1.5 MV/m, respectively. The FLARE FELIX free-electron laser system (Radboud University, The Netherlands) was used as a THz radiation source. The TR effect makes it possible to directly determine the nonlinear susceptibilities of media (including those under conditions of strong absorption) without any reference or optical channel calibration and also without the need of Fourier transform.

Correction to "Terahertz Magnon-Polaritons in TmFeO3".

[This corrects the article DOI: 10.1021/acsphotonics.7b01402.].

Ferrimagnetic spintronics.

Ferrimagnets composed of multiple and antiferromagnetically coupled magnetic elements have attracted much attention recently as a material platform for spintronics. They offer the combined advantages of both ferromagnets and antiferromagnets, namely the easy control and detection of their net magnetization by an external field, antiferromagnetic-like dynamics faster than ferromagnetic dynamics and the potential for high-density devices. This Review summarizes recent progress in ferrimagnetic spintronics, with particular attention to the most-promising functionalities of ferrimagnets, which include their spin transport, spin texture dynamics and all-optical switching.

Ultrafast demagnetization in a ferrimagnet under electromagnetic field funneling.

The quest to improve the density, speed and energy efficiency of magnetic memory storage has led to the exploration of new ways of optically manipulating magnetism at the ultrafast time scale, in particular in ferrimagnetic alloys. While all-optical magnetization switching is well-established on the femtosecond timescale, lateral nanoscale confinement and thus the potential significant reduction of the size of the magnetic element remains an outstanding challenge. Here we employ resonant electromagnetic energy funneling through plasmon nanoantennas to influence the demagnetization dynamics of a ferrimagnetic TbCo alloy thin film. We demonstrate how Ag nanoring-shaped antennas under resonant optical femtosecond pumping reduce the overall demagnetization in the underlying films up to three times compared to non-resonant illumination. We attribute such a substantial reduction to the nanoscale confinement of the demagnetization process. This is qualitatively supported by the electromagnetic simulations that strongly evidence the resonant optical energy-funneling to the nanoscale from the nanoantennas into the ferrimagnetic film. This observation is an important step for reaching deterministic ultrafast all-optical magnetization switching at the nanoscale in such systems, opening a route to develop nanoscale ultrafast magneto-optics.

Fully Controllable Structural Phase Transition in Thermomechanical Molecular Crystals with a Very Small Thermal Hysteresis.

The construction of a practical crystalline molecular machine faces two challenges: to realize a collective molecular movement, and to amplify this movement into a precisely controlled mechanical response in real time and space. Thermosalient single crystals display cooperative molecular movements that are converted to strong macroscopic mechanical responses or shape deformations during temperature-induced structural phase transitions. However, these collective molecular movements are hard to control once initiated, and often feature thermal hystereses that are larger than 10 °C, which greatly hamper their practical applications. Here, it is demonstrated that the phase boundaries of the thermomechanical molecular crystal based on a fluorenone derivative 4-DBpFO can be used to finely control its structural phase transition. When this phase transition is triggered at two opposite crystal faces, it is accompanied by two parallel phase boundaries that can be temperature controlled to move forward, backward, or to halt, benefitting from the stored elastic energy between the parallel boundaries. Moreover, the thermal hysteresis is greatly decreased to 2-3 °C, which allows for circular heating/cooling cycles that can produce a continuous work output.

Halide Perovskites for Nonlinear Optics.

Halide perovskites provide an ideal platform for engineering highly promising semiconductor materials for a wide range of applications in optoelectronic devices, such as photovoltaics, light-emitting diodes, photodetectors, and lasers. More recently, increasing research efforts have been directed toward the nonlinear optical properties of halide perovskites because of their unique chemical and electronic properties, which are of crucial importance for advancing their applications in next-generation photonic devices. Here, the current state of the art in the field of nonlinear optics (NLO) in halide perovskite materials is reviewed. Halide perovskites are categorized into hybrid organic/inorganic and pure inorganic ones, and their second-, third-, and higher-order NLO properties are summarized. The performance of halide perovskite materials in NLO devices such as upconversion lasers and ultrafast laser modulators is analyzed. Several potential perspectives and research directions of these promising materials for nonlinear optics are presented.

Robust thermoelastic microactuator based on an organic molecular crystal.

Mechanically responsive molecular crystals that reversibly change shape triggered by external stimuli are invaluable for the design of actuators for soft robotics, artificial muscles and microfluidic devices. However, their strong deformations usually lead to their destruction. We report a fluorenone derivative (4-DBpFO) showing a strong shear deformation upon heating due to a structural phase transition which is reproducible after more than hundred heating/cooling cycles. Molecular dynamic simulations show that the transition occurs through a nucleation-and-growth mechanism, triggered by thermally induced rotations of the phenyl rings, leading to a rearrangement of the molecular configuration. The applicability as actuator is demonstrated by displacing a micron-sized glass bead over a large distance, delivering a kinetic energy of more than 65 pJ, corresponding to a work density of 270 J kg-1. This material can serve as a prototype structure to direct the development of new types of robust molecular actuators.

Enhanced Second Harmonic Generation from Ferroelectric HfO2-Based Hybrid Metasurfaces.

Integrated nonlinear metasurfaces leading to high-efficiency optical second harmonic generation (SHG) are highly desirable for optical sensing, imaging, and quantum photonic systems. Compared to traditional metal-only metasurfaces, their hybrid counterparts, where a noncentrosymmetric nonlinear photonic material is incorporated in the near-field of a metasurface, can significantly boost SHG efficiency. However, it is difficult to integrate such devices on-chip due to material incompatibilities, thickness scaling challenges, and the narrow band gaps of nonlinear optical materials. Here, we demonstrate significantly enhanced SHG in on-chip integrated metasurfaces by using nanometer thin films of ferroelectric Y:HfO2. This material has the merit of CMOS compatibility, ultraviolet transparency up to 250 nm, and significant scalability down to sub-10 nm when deposited on silicon. We observe a 20-fold magnitude enhancement of the SHG intensity from the hybrid metasurface compared to a bare ferroelectric HfO2 thin film. Moreover, a 3-fold SHG enhancement is observed from the hybrid metasurface compared to a control structure using nonferroelectric HfO2, demonstrating a major contribution to the SHG signal from ferroelectric Y:HfO2. The effective second-order nonlinear optical coefficient χ(2) of Y:HfO2 is determined to be 6.0 ± 0.5 pm/V, which is comparable to other complex nonlinear photonic oxide materials. Our work provides a general pathway to build an efficient on-chip nanophotonic nonlinear light source for SHG using ferroelectric HfO2 thin films.

Chiral Lead Halide Perovskite Nanowires for Second-Order Nonlinear Optics.

Hybrid organic/inorganic lead halide perovskites (LHPs) have recently emerged as extremely promising photonic materials. However, the exploration of their optical nonlinearities has been mainly focused on the third- and higher-order nonlinear optical (NLO) effects. Strong second-order NLO responses are hardly expected from ordinary LHPs due to their intrinsic centrosymmetric structures, but are highly desirable for advancing their applications in the next generation integrated photonic circuits. Here we demonstrate the fabrication of a novel noncentrosymmetric LHP material by introducing chiral amines as the organic component. The nanowires grown from this new LHP material crystallize in a noncentrosymmetric P1 space group and demonstrate highly efficient second harmonic generation (SHG) with high polarization ratios and chiroptical NLO effects. Such a chiral perovskite skeleton could provide a new platform for future engineering of optoelectronic functionalities of hybrid perovskite materials.

Terahertz Magnon-Polaritons in TmFeO3.

Magnon-polaritons are shown to play a dominant role in the propagation of terahertz (THz) waves through TmFeO3 orthoferrite, if the frequencies of the waves are in the vicinity of the quasi-antiferromagnetic spin resonance mode. Both time-domain THz transmission and emission spectroscopies reveal clear beatings between two modes with frequencies slightly above and slightly below this resonance, respectively. Rigorous modeling of the interaction between the spins of TmFeO3 and the THz light shows that the frequencies correspond to the upper and lower magnon-polariton branches. Our findings reveal the previously ignored importance of propagation effects and polaritons in such heavily debated areas as THz magnonics and THz spectroscopy of electromagnons. It also shows that future progress in these areas calls for an interdisciplinary approach at the interface between magnetism and photonics.

Controlling the Growth of Molecular Crystal Aggregates with Distinct Linear and Nonlinear Optical Properties.

Two novel donor-acceptor molecules, 2,7-diphenylbenzo[1,2-b:4,3-b']difuran-4,5-dicarbonitrile and 2,7-bis(4-methoxyphenyl)benzo[1,2-b:4,3-b']difuran-4,5-dicarbonitrile containing cyano group as the electron acceptor, were synthesized. Their single-crystal structures, molecular packing, and self-assembly behaviors were also investigated. By simple solvent evaporation techniques, these compounds self-assemble into various low-dimensional microstructures that demonstrate distinctive nonlinear optical properties depending on the orientations of their transition dipoles. This study highlights the importance of the transition dipole moment in the construction of low-dimensional molecular materials with highly efficient nonlinear optical properties.

All-optical observation and reconstruction of spin wave dispersion.

To know the properties of a particle or a wave, one should measure how its energy changes with its momentum. The relation between them is called the dispersion relation, which encodes essential information of the kinetics. In a magnet, the wave motion of atomic spins serves as an elementary excitation, called a spin wave, and behaves like a fictitious particle. Although the dispersion relation of spin waves governs many of the magnetic properties, observation of their entire dispersion is one of the challenges today. Spin waves whose dispersion is dominated by magnetostatic interaction are called pure-magnetostatic waves, which are still missing despite of their practical importance. Here, we report observation of the band dispersion relation of pure-magnetostatic waves by developing a table-top all-optical spectroscopy named spin-wave tomography. The result unmasks characteristics of pure-magnetostatic waves. We also demonstrate time-resolved measurements, which reveal coherent energy transfer between spin waves and lattice vibrations.

High-Efficiency Second-Harmonic Generation from Hybrid Light-Matter States.

We report a novel approach to modify the second order nonlinear optical (NLO) susceptibility of organic nanofiber crystals by hybridization with the optical modes of microcavities in the strong coupling regime. The wavelength dependence of the SHG efficiency displays two intense peaks corresponding to the so-formed light-matter hybrid states. Our results demonstrate an enhancement of the resonant SHG efficiency of the lower polariton by 2 orders of magnitude for the collectively coupled molecules as compared to that of the same material outside the microcavity. This study is a proof of principle that opens a new direction for NLO of organic materials in subwavelength resonators.

Colossal magneto-optical modulation at terahertz frequencies by counterpropagating femtosecond laser pulses in Tb3Ga5O12.

Single-frequency terahertz modulation of the magneto-optical Faraday effect with a record amplitude of the polarization rotation of ∼0.5° is achieved using a slab of the etalon Faraday rotator crystal Tb3Ga5O12. The modulation is the result of the interaction of two counterpropagating laser pulses via the optical Kerr effect. The frequency of the modulation is determined by the applied magnetic field and is continuously tunable in a terahertz frequency range between 0 and 0.7 THz.

Switching of chiral magnetic skyrmions by picosecond magnetic field pulses via transient topological states.

Magnetic chiral skyrmions are vortex like spin structures that appear as stable or meta-stable states in magnetic materials due to the interplay between the symmetric and antisymmetric exchange interactions, applied magnetic field and/or uniaxial anisotropy. Their small size and internal stability make them prospective objects for data storage but for this, the controlled switching between skyrmion states of opposite polarity and topological charge is essential. Here we present a study of magnetic skyrmion switching by an applied magnetic field pulse based on a discrete model of classical spins and atomistic spin dynamics. We found a finite range of coupling parameters corresponding to the coexistence of two degenerate isolated skyrmions characterized by mutually inverted spin structures with opposite polarity and topological charge. We demonstrate how for a wide range of material parameters a short inclined magnetic field pulse can initiate the reliable switching between these states at GHz rates. Detailed analysis of the switching mechanism revealed the complex path of the system accompanied with the excitation of a chiral-achiral meron pair and the formation of an achiral skyrmion.

Spectrally resolved optical probing of laser induced magnetization dynamics in bismuth iron garnet.

The spectrally resolved magnetization dynamics in bismuth iron garnet shows a fluence dependent light induced modification of the magneto-optical Faraday spectrum. It is demonstrated that the relative contributions from the tetrahedral and octahedral iron sites to the Faraday spectrum change due to the impact of the pump pulse. This change explains the observed deviation from a linear dependence of the amplitude of the oscillations on the fluence, as expected for the inverse Faraday effect.

Electric field generation of Skyrmion-like structures in a nematic liquid crystal.

Skyrmions are particle-like topological objects that are increasingly drawing attention in condensed matter physics, where they are connected to inversion symmetry breaking and chirality. Here we report the generation of stable Skyrmion-like structures in a thin nematic liquid crystal film on chemically patterned patchy surfaces. Using the interplay of material elasticity and surface boundary conditions, we use a strong electric field to quench the nematic liquid crystal from a fully aligned phase to vortex-like nematic liquid crystal structures, centered on patterned patches, which carry two different sorts of topological defects. Numerical calculations reveal that these are Skyrmion-like structures, seeded from the surface boojum topological defects and swirling towards the second confining surface. These observations, supported by numerical methods, demonstrate the possibility to generate, manipulate and study Skyrmion-like objects in nematic liquid crystals on patterned surfaces.

Nanoscale Confinement of All-Optical Magnetic Switching in TbFeCo--Competition with Nanoscale Heterogeneity.

Single femtosecond optical laser pulses, of sufficient intensity, are demonstrated to reverse magnetization in a process known as all-optical switching. Gold two-wire antennas are placed on the all-optical switching film TbFeCo. These structures are resonant with the optical field, and they create a field enhancement in the near-field which confines the area where optical switching can occur. The magnetic switching that occurs around and below the antenna is imaged using resonant X-ray holography and magnetic circular dichroism. The results not only show the feasibility of controllable switching with antenna assistance but also demonstrate the highly inhomogeneous nature of the switching process, which is attributed to the process depending on the material's heterogeneity.

Channeling Vibrational Energy To Probe the Electronic Density of States in Metal Clusters.

We investigate the electronic density of states (DOS) of isolated neutral cobalt clusters by probing the temperature-modulated population of electronic states through UV photoionization. The temperature is controlled via resonant excitation of lattice vibrations using the free-electron laser FELICE, after which the vibrational and electronic systems equilibrate through the electron-phonon coupling, redistributing the population of electronic states. The data are analyzed by surface photoemission theory, modified to incorporate the realistic DOS.