Correction: Ultrafast switching to zero field topological spin textures in ferrimagnetic TbFeCo films.

Correction for 'Ultrafast switching to zero field topological spin textures in ferrimagnetic TbFeCo films' by Kaixin Zhu et al., Nanoscale, 2024, 16, 3133-3143, https://doi.org/10.1039/D3NR04529C.

Spatiotemporal Visualization of Photogenerated Carriers on an Avalanche Photodiode Surface Using Ultrafast Scanning Electron Microscopy.

The spatiotemporal evolution of photogenerated charge carriers on surfaces and at interfaces of photoactive materials is an important issue for understanding fundamental physical processes in optoelectronic devices and advanced materials. Conventional optical probe-based microscopes that provide indirect information about the dynamic behavior of photogenerated carriers are inherently limited by their poor spatial resolution and large penetration depth. Herein, we develop an ultrafast scanning electron microscope (USEM) with a planar emitter. The photoelectrons per pulse in this USEM can be two orders of magnitude higher than that of a tip emitter, allowing the capture of high-resolution spatiotemporal images. We used the contrast change of the USEM to examine the dynamic nature of surface carriers in an InGaAs/InP avalanche photodiode (APD) after femtosecond laser excitation. It was observed that the photogenerated carriers showed notable longitudinal drift, lateral diffusion, and carrier recombination associated with the presence of photovoltaic potential at the surface. This work demonstrates an in situ multiphysics USEM platform with the capability to stroboscopically record carrier dynamics in space and time.

Ultrafast switching to zero field topological spin textures in ferrimagnetic TbFeCo films.

The capability of femtosecond (fs) laser pulses to manipulate topological spin textures on a very short time scale is sparking considerable interest. This article presents the creation of high density zero field topological spin textures by fs laser excitation in ferrimagnetic TbFeCo amorphous films. The topological spin textures are demonstrated to emerge under fs laser pulse excitation through a unique ultrafast nucleation mechanism, rather than thermal effects. Notably, large intrinsic uniaxial anisotropy could substitute the external magnetic field for the creation and stabilization of topological spin textures, which is further verified by the corresponding micromagnetic simulation. The ultrafast switching between topological trivial and nontrivial magnetic states is realized at an optimum magnitude of magnetic field and laser fluence. Our results would broaden the options to generate zero-field topological spin textures from versatile magnetic states and provides a new perspective for ultrafast switching of 0/1 magnetic states in spintronic devices.

Simulation of ultrafast electron diffraction intensity under coherent acoustic phonons.

Ultrafast electron diffraction has been proven to be a powerful tool for the study of coherent acoustic phonons owing to its high sensitivity to crystal structures. However, this sensitivity leads to complicated behavior of the diffraction intensity, which complicates the analysis process of phonons, especially higher harmonics. Here, we theoretically analyze the effects of photoinduced coherent transverse and longitudinal acoustic phonons on electron diffraction to provide a guide for the exploitation and modulation of coherent phonons. The simulation of the electron diffraction was performed in 30-nm films with different optical penetration depths based on the atomic displacements obtained by solving the wave equation. The simulation results exhibit a complex relationship between the frequencies of the phonons and diffraction signals, which highly depends on the laser penetration depth, sample thickness, and temporal stress distribution. In addition, an intensity decomposition method is proposed to account for the in-phase oscillation and high harmonics caused by inhomogeneous excitation. These results can provide new perspectives and insights for a comprehensive and accurate understanding of the lattice response under coherent phonons.

Efficiently accelerated free electrons by metallic laser accelerator.

Strong electron-photon interactions occurring in a dielectric laser accelerator provide the potential for development of a compact electron accelerator. Theoretically, metallic materials exhibiting notable surface plasmon-field enhancements can possibly generate a high electron acceleration capability. Here, we present a design for metallic material-based on-chip laser-driven accelerators that show a remarkable electron acceleration capability, as demonstrated in ultrafast electron microscopy investigations. Under phase-matching conditions, efficient and continuous acceleration of free electrons on a periodic nanostructure can be achieved. Importantly, an asymmetric spectral structure in which the vast majority of the electrons are in the energy-gain states has been obtained by means of a periodic bowtie-structure accelerator. Due to the presence of surface plasmon enhancement and nonlinear optical effects, the maximum acceleration gradient can reach as high as 0.335 GeV/m. This demonstrates that metallic laser accelerator could provide a way to develop compact accelerators on chip.

Critical Role Played by Interface Engineering in Weakening Thickness Dependence of Superconducting and Structural Properties of FeSe0.5Te0.5-Coated Conductors.

Increasing the thickness of a superconducting layer and simultaneously reducing the thickness effect in iron-based superconducting coated conductors are particularly essential for improving the critical current Ic. Here, for the first time, we have deposited high-performance FeSe0.5Te0.5 (FST) superconducting films up to 2 µm on LaMnO3-buffered metal tapes by pulsed laser deposition. An interface engineering strategy, alternating growth of a 10 nm-thick nonsuperconducting FST seed layer and a 400 nm-thick FST superconducting layer, was employed to guarantee the crystalline quality of the films with thicknesses of the order of micrometers, resulting in a highly biaxial texture with grain boundary misorientation angle less than the critical value θc ∼ 9°. Moreover, the thickness effect, that the critical current density (Jc) shows a clear dependence on thickness as in cuprates, is reduced by the interface engineering. Also, the maximum Jc was found for a 400 nm-thick film with 1.3 MA/cm2 in self-field at 4.2 K and 0.71 MA/cm2 (H∥ab) and 0.50 MA/cm2 (H∥c) at 9 T. Anisotropic Ginzburg-Landau scaling indicates that the major pinning centers vary from correlated to uncorrelated as the film thickness increases, while the thickness effect is most likely related to the weakening of flux pinning by the fluctuation of charge-carrier mean free path (δl) and strengthening of flux pinning caused by the variation of superconducting transition temperature (δTc) due to off-stoichiometry with thickness.

Magnetotransport property of oxygen-annealed Fe1+yTe thin films.

Fe-based superconductors are one of the current research focuses. FeTe is unique in the series of FeSe1-xTex, since it is nonsuperconducting near the FeTe side in the phase diagram in contrast to the presence of superconductivity in other region. However, FeTe thin films become superconducting after oxygen annealing and the mechanism remains elusive. Here, we report the temperature dependences of resistivity, Hall effect and magnetoresistance (MR) of a series of FeTe thin films with different amounts of excess Fe and oxygen. These properties show dramatic changes with excess Fe and oxygen incorporation. We found the Hall coefficients are positive for the oxygen-annealed samples, in contrast to the transition from positive to negative below 50 K for the vacuum-annealed samples. For all samples, both the resistivity and Hall coefficient show a dramatic drop, respectively, at around 50 K-75 K, implying coexistence of superconductivity and antiferromagnetic order for the oxygen-annealed samples. The vacuum-annealed samples show both positive and negative values of MR depending on temperature, while negative MR dominates for the oxygen-annealed samples. We also found that oxygen annealing reduces the excess Fe in FeTe, which has been neglected before. The results are discussed in terms of several contributions, and a comparison is made between the oxygen-annealed FeTe thin films and FeSe1-xTex. This work is helpful for shedding light on the understanding of oxygen-annealed FeTe thin films.

Enhancement of lattice dynamics by an azimuthal surface plasmon on the femtosecond time scale in multi-walled carbon nanotubes.

Plasmon-enhanced light-matter interactions have been widely investigated in the past decades. Here, we report surface plasmon-enhanced structural dynamics in multi-walled carbon nanotubes. The optical polarization dependent dynamic properties of multi-walled carbon nanotubes are investigated using ultrafast transmission electron microscopy. Lattice contractions in the femtosecond time regime are observed upon excitation of the azimuthal plasmon by light polarized perpendicular to the tubular axis. The polarization dependence of the plasmon near field was examined using photon-induced near-field electron microscopy. The lattice changes resulting from the azimuthal plasmon enhance ultrafast alterations in both localized evanescent fields and the collective charge excitation, which play critical roles governing the light-matter interaction. These results suggest that the ultrafast responses of lattice degrees of freedom in nanomaterials could be essential for understanding the mechanism of surface plasmon enhanced effects.

Nanoscale Visualization of a Photoinduced Plasmonic Near-Field in a Single Nanowire by Free Electrons.

Swift electrons can undergo inelastic interactions not only with electrons but also with near-fields, which may result in an energy loss or gain. Developments in photon-induced near-field electron microscopy (PINEM) enable direct imaging of the plasmon near-field distribution with nanometer resolution. Here, we report an analysis of the surface plasmonic near-field structure based on PINEM observations of silver nanowires. Single-photon order-selected electron images revealed the wavelike and banded structure of electric equipotential regions for a confined near-field integral associated with typical absorption of photon quanta (nℏω). Multimodal plasmon oscillations and second-harmonic generation were simultaneously observed, and the polarization dependence of plasmon wavelength and symmetry properties were analyzed. Based on advanced imaging techniques, our work has implications for future studies of the localized-field structures at interfaces and visualization of novel phenomena in nanostructures, nanosensors, and plasmonic devices.

Microstructure of quasi-one-dimensional superconductor KCr3As3prepared by K-ion deintercalation.

The microstructure of quasi-one-dimensional KCr3As3(133) superconductors, which were prepared by chemical cation deintercalation from their counterpart K2Cr3As3(233) compounds, are investigated using scanning transmission electron microscopy. The nominal KCr3As3crystals generally exhibit irregular nanoscale 133-phase domains accompanied by an amorphous As-deficient phase and cracks as a result of alkali cation deintercalation processes. Analysis of local defective structures reveals the existence of an intermediate state in the transformation from 233 to 133 phase and a possible K-deficient 233-type structure as a nanoscale cluster. Our microscopic investigations offer insight into the microstructure of KCr3As3and the alkali metal cation deintercalation processes.

Electric-field control of skyrmions in multiferroic heterostructure via magnetoelectric coupling.

Room-temperature skyrmions in magnetic multilayers are considered to be promising candidates for the next-generation spintronic devices. Several approaches have been developed to control skyrmions, but they either cause significant heat dissipation or require ultrahigh electric fields near the breakdown threshold. Here, we demonstrate electric-field control of skyrmions through strain-mediated magnetoelectric coupling in ferromagnetic/ferroelectric multiferroic heterostructures. We show the process of non-volatile creation of multiple skyrmions, reversible deformation and annihilation of a single skyrmion by performing magnetic force microscopy with in situ electric fields. Strain-induced changes in perpendicular magnetic anisotropy and interfacial Dzyaloshinskii-Moriya interaction strength are characterized experimentally. These experimental results, together with micromagnetic simulations, demonstrate that strain-mediated magnetoelectric coupling (via strain-induced changes in both the perpendicular magnetic anisotropy and interfacial Dzyaloshinskii-Moriya interaction is responsible for the observed electric-field control of skyrmions. Our work provides a platform to investigate electric-field control of skyrmions in multiferroic heterostructures and paves the way towards more energy-efficient skyrmion-based spintronics.

Growth of High-Quality Superconducting FeSe0.5Te0.5 Films on Pb(Mg1/3Nb2/3)0.7Ti0.3O3 and Electric-Field Modulation of Superconductivity.

Heterostructures composed of superconductor and ferroelectrics (SC/FE) are very important for manipulating the superconducting property and applications. However, growth of high-quality superconducting iron chalcogenide films is challenging because of their volatility and FE substrate with rough surface and large lattice mismatch. Here, we report a two-step growth approach to get high-quality FeSe0.5Te0.5 (FST) films on FE Pb(Mg1/3Nb2/3)0.7Ti0.3O3 with large lattice mismatch, which show superconductivity at only around 10 nm. Through a systematic study of structural and electric transport properties of samples with different thicknesses, a mechanism to grow high-quality FST is discovered. Moreover, electric-field-induced remarkable change of Tc (superconducting transition temperature) is demonstrated in a 20 nm FST film. This work paves the way to grow high-quality films which contain volatile element and have large lattice mismatch with the substrate. It is also helpful for manipulating the superconducting property in SC/FE heterostructures.

Development of analytical ultrafast transmission electron microscopy based on laser-driven Schottky field emission.

A new design scheme for ultrafast transmission electron microscopy (UTEM) has been developed based on a Schottky-type field emission gun (FEG) at the Institute of Physics, Chinese Academy of Sciences (IOP CAS). In this UTEM setup, electron pulse emission is achieved by integrating a laser port between the electron gun and the column and the resulting microscope can operate in either continuous or pulsed mode. In pulsed mode, the optimized electron beam properties are an energy width of ~0.65 eV, micrometer-scale coherence lengths and sub-picosecond pulse durations. The potential applications of this UTEM, which include electron diffraction, high-resolution imaging, electron energy loss spectroscopy, and photon-induced near-field electron microscopy, are demonstrated using ultrafast electron pulses. Furthermore, we use a nanosecond laser (~10 ns) to show that the laser-driven FEG can support high-quality TEM imaging and electron holography when using a stroboscopic configuration. Our results also indicate that FEG-based ultrafast electron sources may enable high-performance analytical UTEM.

Ultrafast lattice and electronic dynamics in single-walled carbon nanotubes.

Understanding the photoinduced ultrafast structural transitions and electronic dynamics in single-walled carbon nanotubes (SWCNTs) is important for the development of SWCNT-based optoelectronic devices. In this study, we conducted femtosecond-resolved electron diffraction and electron energy-loss spectroscopy (EELS) measurements on SWCNTs using ultrafast transmission electron microscopy. The experimental results demonstrated that dominant time constants of the dynamic processes were ∼1.4 ps for electron-driven lattice expansion, ∼17.4 ps for thermal phonon-driven lattice expansion associated with electron-phonon coupling. The time-resolved EELS measurements clearly revealed a notable red shift of plasmon peaks by ∼100 meV upon femtosecond laser excitation. Different features of charge carrier excitation and relaxation were carefully discussed in correlation with the lattice dynamics and photoinduced absorption signals of SWCNTs. Our results provide a comprehensive understanding of the ultrafast dynamics in SWCNTs and powerful techniques to characterize the dynamics of low-dimensional structures.

Lattice Dynamics and Contraction of Energy Bandgap in Photoexcited Semiconducting Boron Nitride Nanotubes.

Structural dynamics and changes in electronic structures driven by photoexcited carriers are critical issues in both semiconducting and optoelectronic nanodevices. Herein, a phase diagram for the transient states and relevant dynamic processes in multiwalled boron nitride nanotubes (BNNTs) has been extensively studied for a full reversible cycle after a fs-laser excitation in ultrafast TEMs, and the significant structural features and evolution of electronic natures have been investigated using pulsed electron diffraction and femtosecond-resolved electron energy-loss spectroscopy (EELS). It is revealed that nonthermal anisotropic alterations of the lattice apparently precede the phonon-driven thermal transients along the radial and axial directions. Ab initio calculations support these findings and show that electrons excited from the π to π* orbitals in the BN nanotubes weaken the intralayer bonds while strengthening the interlayer bonds along the radial direction. Importantly, time-resolved EELS measurements show contraction of the energy bandgap after fs-laser excitation associated with nonthermal structural transients. This fact verifies that laser-induced bandgap renormalization in semiconductors can essentially be correlated with both the rapid processes of excited carriers and nonthermal lattice evolution.

Hidden CDW states and insulator-to-metal transition after a pulsed femtosecond laser excitation in layered chalcogenide 1T-TaS2- x Se x.

The hidden (H) quantum state in 1T-TaS2 has sparked considerable interest in the field of correlated electron systems. Here, we investigate ultrafast switches to stable H charge density wave (H-CDW) states observed in 1T-TaS2-x Se x , with x = 0 and 0.5 crystals, upon excitation with a single femtosecond laser pulse. In situ cooling transmission electron microscopy observations, initiated by a single femtosecond laser pumping with a low fluence, reveal a clear transition from a commensurate CDW phase (qC) to a new CDW order with qH = (1 - δ)qC for the H-CDW state (δ = 1/9) accompanied by an evident phase separation. H-CDW domain relaxation then occurs and yields a stable metallic phase under a high-fluence excitation. Furthermore, electrical resistivity measurements show that the notable drop in x = 0 and 0.5 samples associated with the appearance of H-CDW states depend on laser fluence and temperature. These results potentially provide a new perspective on the photodoping mechanism for the emergence of H-CDW states in the 1T-TaS2-x Se x family.

Quantification of Magnetic Surface and Edge States in an FeGe Nanostripe by Off-Axis Electron Holography.

Whereas theoretical investigations have revealed the significant influence of magnetic surface and edge states on Skyrmonic spin texture in chiral magnets, experimental studies of such chiral states remain elusive. Here, we study chiral edge states in an FeGe nanostripe experimentally using off-axis electron holography. Our results reveal the magnetic-field-driven formation of chiral edge states and their penetration lengths at 95 and 240 K. We determine values of saturation magnetization M_{S} by analyzing the projected in-plane magnetization distributions of helices and Skyrmions. Values of M_{S} inferred for Skyrmions are lower by a few percent than those for helices. We attribute this difference to the presence of chiral surface states, which are predicted theoretically in a three-dimensional Skyrmion model. Our experiments provide direct quantitative measurements of magnetic chiral boundary states and highlight the applicability of state-of-the-art electron holography for the study of complex spin textures in nanostructures.

Cooperative inter- and intra-layer lattice dynamics of photoexcited multi-walled carbon nanotubes studied by ultrafast electron diffraction.

Optical tuning and probing ultrafast structural response of nanomaterials driven by electronic excitation constitute a challenging but promising approach for understanding microscopic mechanisms and applications in microelectromechanical systems and optoelectrical devices. Here we use pulsed electron diffraction in a transmission electron microscope to investigate laser-induced tubular lattice dynamics of multi-walled carbon nanotubes (MWCNTs) with varying laser fluence and initial specimen temperature. Our photoexcitation experiments demonstrate cooperative and inverse collective atomic motions in intralayer and interlayer directions, whose strengths and rates depend on pump fluence. The electron-driven and thermally driven structural responses with opposite amplitudes cause a crossover between intralayer and interlayer directions. Our ab initio calculations support these findings and reveal that electrons excited from π to π* orbitals in a carbon tube weaken the intralayer bonds while strengthening the interlayer bonds along the radial direction. Moreover, by probing the structural dynamics of MWCNTs at initial temperatures of 300 and 100 K, we uncover the concomitance of thermal and nonthermal dynamical processes and their mutual influence in MWCNTs. Our results illustrate the nature of electron-driven nonthermal process and electron-phonon thermalization in the MWCNTs, and bear implications for the intricate energy conversion and transfer in materials at the nanoscale.

Direct Observation of Inner-Layer Inward Contractions of Multiwalled Boron Nitride Nanotubes upon in Situ Heating.

In situ heating transmission electron microscopy observations clearly reveal remarkable interlayer expansion and inner-layer inward contraction in multi-walled boron nitride nanotubes (BNNTs) as the specimen temperature increases. We interpreted the observed inward contraction as being due to the presence of the strong constraints of the outer layers on radial expansion in the tubular structure upon in situ heating. The increase in specimen temperature upon heating can create pressure and stress toward the tubular center, which drive the lattice motion and yield inner diameter contraction for the multi-walled BNNTs. Using a simple model involving a wave-like pattern of layer-wise distortion, we discuss these peculiar structural alterations and the anisotropic thermal expansion properties of the tubular structures. Moreover, our in situ atomic images also reveal Russian-doll-type BN nanotubes, which show anisotropic thermal expansion behaviors.

Ultrafast structural dynamics of boron nitride nanotubes studied using transmitted electrons.

We investigate the ultrafast structural dynamics of multi-walled boron nitride nanotubes (BNNTs) upon femtosecond optical excitation using ultrafast electron diffraction in a transmission electron microscope. Analysis of the time-resolved (100) and (002) diffraction profiles reveals highly anisotropic lattice dynamics of BNNTs, which can be attributed to the distinct nature of the chemical bonds in the tubular structure. Moreover, the changes in (002) diffraction positions and intensities suggest that the lattice response of BNNTs to the femtosecond laser excitation involves a fast and a slow lattice dynamic process. The fast process with a time constant of about 8 picoseconds can be understood to be a result of electron-phonon coupling, while the slow process with a time constant of about 100 to 300 picoseconds depending on pump laser fluence is tentatively associated with an Auger recombination effect. In addition, we discuss the power-law relationship of a three-photon absorption process in the BNNT nanoscale system.