Time-resolved Photoemission Electron Microscopy Research Articles

Unraveling Spatially Heterogeneous Ultrafast Carrier Dynamics of Single-Layer WSe2 by Femtosecond Time-Resolved Photoemission Electron Microscopy.

Studies of the ultrafast carrier dynamics of transition metal dichalcogenides have employed spatially averaged measurements, which obfuscate the rich variety of dynamics that originate from the structural heterogeneity of these materials. Here, we employ femtosecond time-resolved photoemission electron microscopy (TR-PEEM) with sub-80 nm spatial resolution to image the ultrafast subpicosecond to picosecond carrier dynamics of monolayer tungsten diselenide (WSe2). The dynamics observed following 2.41 eV pump and 3.61 eV probe occurs on two distinct time scales. The 0.1 ps process is assigned to electron cooling via intervalley scattering, whereas the picosecond dynamics is attributed to exciton-exciton annihilation. The 70 fs decay dynamics observed at negative time delay reflects electronic relaxation from the Γ point. Analysis of the TR-PEEM data furnishes the spatial distributions of the various time constants within a single WSe2 flake. The spatial heterogeneity of the lifetime maps is consistent with increased disorder along the edges of the flake and the presence of nanoscale charge puddles in the interior. Our results indicate the need to go beyond spatially averaged time-resolved measurements to understand the influence of structural heterogeneities on the elementary carrier dynamics of two-dimensional materials.

Cavity-assisted ultrafast long-range periodic energy transfer between plasmonic nanoantennas

Radiationless energy transfer is at the core of diverse phenomena, such as light harvesting in photosynthesis(1), energy-transfer-based microspectroscopies(2), nanoscale quantum entanglement(3) and photonic-mode hybridization(4). Typically, the transfer is efficient only for separations that are much shorter than the diffraction limit. This hampers its application in optical communication and quantum information processing, which require spatially selective addressing. Here, we demonstrate highly efficient radiationless coherent energy transfer over a distance of twice the excitation wavelength by combining localized and delocalized(5) plasmonic modes. Analogous to the Tavis-Cummings model, two whispering-gallery-mode antennas(6) placed in the foci of an elliptical plasmonic cavity(7) fabricated from single-crystal gold plates act as a pair of oscillators coupled to a common cavity mode. Time-resolved two-photon photoemission electron microscopy (TR 2P-PEEM) reveals an ultrafast long-range periodic energy transfer in accordance with the simulations. Our observations open perspectives for the optimization and tailoring of mesoscopic energy transfer and long-range quantum emitter coupling.

Ultrafast Microscopy: Imaging Light with Photoelectrons on the Nano-Femto Scale.

Experimental methods for ultrafast microscopy are advancing rapidly. Promising methods combine ultrafast laser excitation with electron-based imaging or rely on super-resolution optical techniques to enable probing of matter on the nano-femto scale. Among several actively developed methods, ultrafast time-resolved photoemission electron microscopy provides several advantages, among which the foremost are that time resolution is limited only by the laser source and it is immediately capable of probing of coherent phenomena in solid-state materials and surfaces. Here we present recent progress in interference imaging of plasmonic phenomena in metal nanostructures enabled by combining a broadly tunable femtosecond laser excitation source with a low-energy electron microscope.

Revealing the subfemtosecond dynamics of orbital angular momentum in nanoplasmonic vortices.

The ability of light to carry and deliver orbital angular momentum (OAM) in the form of optical vortices has attracted much interest. The physical properties of light with a helical wavefront can be confined onto two-dimensional surfaces with subwavelength dimensions in the form of plasmonic vortices, opening avenues for thus far unknown light-matter interactions. Because of their extreme rotational velocity, the ultrafast dynamics of such vortices remained unexplored. Here we show the detailed spatiotemporal evolution of nanovortices using time-resolved two-photon photoemission electron microscopy. We observe both long- and short-range plasmonic vortices confined to deep subwavelength dimensions on the scale of 100 nanometers with nanometer spatial resolution and subfemtosecond time-step resolution. Finally, by measuring the angular velocity of the vortex, we directly extract the OAM magnitude of light.

半導体表面における光励起キャリアダイナミクスの時間・空間分解計測

A system for time-resolved photoemission electron microscopy (TR-PEEM) conducted with femtosecond laser pulses has been developed to explore the photogenerated electron dynamics on semiconductor surfaces. Attained space and time resolutions were 100 nm and 100 fs, respectively. The present manuscript introduces the TR-PEEM system, and also reports the observation of different photogenerated electron lifetimes in different nanoscale structural defects randomly distributed on a semiconductor surface. The results were explained based on Schockley-Read-Hall (SRH) model relating the carrier recombination time and the defect state density. The defect state density in each defect was successfully estimated.

Enhanced Propagating Surface Plasmon Signal Detection

Overcoming the dissipative nature of propagating surface plasmons (PSPs) is a prerequisite to realizing functional plasmonic circuitry, in which large-bandwidth signals can be manipulated over length scales far below the diffraction limit of light. To this end, we report on a novel PSP-enhanced signal detection technique achieved in an all-metallic substrate. We take advantage of two strategically spatiotemporally separated phase-locked femtosecond laser pulses, incident onto lithographically patterned PSP coupling structures. We follow PSP propagation with joint femtosecond temporal and nanometer spatial resolution in a time-resolved nonlinear photoemission electron microscopy scheme. Initially, a PSP signal wave packet is launched from a hole etched into the silver surface from where it propagates through an open trench structure and is decoded through the use of a timed probe pulse. FDTD calculations demonstrate that PSP signal waves may traverse open trenches in excess of 10 μm in diameter, thereby al...

Determination of local optical response functions of nanostructures with increasing complexity by using single and coupled Lorentzian oscillator models

We reconstruct the optical response of nanostructures of increasing complexity by fitting interferometric time-resolved photoemission electron microscopy (PEEM) data from an ultrashort (21 fs) laser excitation source with different harmonic oscillator-based models. Due to its high spatial resolution of ~40 nm, PEEM is a true near-field imaging system and enables in normal incidence mode a mapping of plasmon polaritons and an intuitive interpretation of the plasmonic behaviour. Using an actively stabilized Mach–Zehnder interferometer, we record two-pulse correlation signals with 50 as time resolution that contain information about the temporal plasmon polariton evolution. Spectral amplitude and phase of excited plasmon polaritons are extracted from the recorded phase-resolved interferometric two-pulse correlation traces. We show that the optical response of a plasmon polariton generated at a gold nanoparticle can be reconstructed from the interferometric two-pulse correlation signal using a single harmonic oscillator model. In contrast, for a corrugated silver surface, a system with increased plasmonic complexity, in general an unambiguous reconstruction of the local optical response based on coupled and uncoupled harmonic oscillators, fails. Whereas for certain local responses different models can be discriminated, this is impossible for other positions. Multidimensional spectroscopy offers a possibility to overcome this limitation.

Dissecting the Few-Femtosecond Dephasing Time of Dipole and Quadrupole Modes in Gold Nanoparticles Using Polarized Photoemission Electron Microscopy.

Dipole and quadrupole modes are the two lowest orders of localized surface plasmon resonance (LSPR) eigenmodes in metallic nanoparticles. Of these two modes, the quadrupole mode is forbidden for symmetric metallic nanoparticles excited by linearly polarized light at normal incidence. Here, we demonstrate excitation of the quadrupole mode in symmetrical gold (Au) nanoblocks shined with s-polarized light at oblique incidence. In particular, we probe the near-field LSPR in Au nanoblocks using photoemission electron microscopy (PEEM) and find that at oblique incidence, the dipole and quadrupole modes can be selectively excited, in terms of near-field enhancement, by manipulating the light polarization state. More importantly, by time-resolved PEEM measurements, we experimentally demonstrate that the quadrupole mode in symmetrical Au nanoblocks has longer dephasing time than that of the dipole mode.

Lifetimes of photogenerated electrons on a GaAs surface affected by nanostructural defects

The recombination dynamics of photogenerated carriers on temporal and spatial scales of 100 fs and 100 nm, respectively, on an inhomogeneous GaAs surface with structural defects was investigated using time-resolved photoemission electron microscopy with femtosecond laser pulses. The observed photocarrier lifetimes (τ) ranged from subpicoseconds to picoseconds at isolated structural defects and were inversely proportional to the photoemission intensity at each defect. We concluded that τ corresponds to the carrier trapping time to midgap defect states and estimated the density of the midgap states at each defect on the basis of the relation between τ and the photoemission intensity.

Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna.

The local enhancement of few-cycle laser pulses by plasmonic nanostructures opens up for spatiotemporal control of optical interactions on a nanometer and few-femtosecond scale. However, spatially resolved characterization of few-cycle plasmon dynamics poses a major challenge due to the extreme length and time scales involved. In this Letter, we experimentally demonstrate local variations in the dynamics during the few strongest cycles of plasmon-enhanced fields within individual rice-shaped silver nanoparticles. This was done using 5.5 fs laser pulses in an interferometric time-resolved photoemission electron microscopy setup. The experiments are supported by finite-difference time-domain simulations of similar silver structures. The observed differences in the field dynamics across a single particle do not reflect differences in plasmon resonance frequency or dephasing time. They instead arise from a combination of retardation effects and the coherent superposition between multiple plasmon modes of the particle, inherent to a few-cycle pulse excitation. The ability to detect and predict local variations in the few-femtosecond time evolution of multimode coherent plasmon excitations in rationally synthesized nanoparticles can be used in the tailoring of nanostructures for ultrafast and nonlinear plasmonics.

Probing of Ultrafast Plasmon Dynamics on Gold Bowtie Nanostructure Using Photoemission Electron Microscopy**Supported by the National Basic Research Program of China under Grant No 2013CB922404, the National Natural Science Foundation of China under Grant Nos 11474040 11274053, 11474039 and 61178022, and the Project under Grant No 14KP007.

We report the direct imaging of plasmon on the tips of nano-prisms in a bowtie structure excited by 7 fs laser pulses and probing of ultrafast plasmon dynamics by combining the pump-probe technology with three-photon photoemission electron microscopy. Different photoemission patterns induced by the plasmon effect are observed when the bowties are excited by s- and p-polarized femtosecond laser pulses. A series of images of the evolution of local surface plasmon modes on different tips of the bowtie are obtained by the time-resolved three-photon photoemission electron microscopy, and the result discloses that plasmon excitation is dominated by the interference of the pump and probe pulses within the first 13 fs of the delay time, and thereafter the individual plasmon starts to oscillate on its own characteristic resonant frequencies.

Real-time observation of domain fluctuations in a two-dimensional magnetic model system.

Domain patterns of perpendicularly magnetized ultra-thin ferromagnetic films are often determined by the competition of the short range but strong exchange interaction favouring ferromagnetic alignment of magnetic moments and the long range but weak antiferromagnetic dipolar interaction. Detailed phase diagrams of the resulting stripe domain patterns have been evaluated in recent years; however, the domain fluctuations in these pattern forming systems have not been studied in great detail so far. Here we show that domain fluctuations can be observed in ultra-thin two-dimensional ferromagnetic Fe/Ni/Cu(001) films with perpendicular magnetization in the stripe domain phase. Non-stroboscopic time-resolved threshold photoemission electron microscopy with high temporal resolution allows analysing the dynamic fingerprint of the topological excitations in the nematic domain phase. Furthermore, proliferation of domain ending defects in the vicinity of the spin reorientation transition is witnessed.

Ultrafast imaging of surface plasmons propagating on a gold surface.

We record time-resolved nonlinear photoemission electron microscopy (tr-PEEM) images of propagating surface plasmons (PSPs) launched from a lithographically patterned rectangular trench on a flat gold surface. Our tr-PEEM scheme involves a pair of identical, spatially separated, and interferometrically locked femtosecond laser pulses. Power-dependent PEEM images provide experimental evidence for a sequential coherent nonlinear photoemission process, in which one laser source launches a PSP through a linear interaction, and the second subsequently probes the PSP via two-photon photoemission. The recorded time-resolved movies of a PSP allow us to directly measure various properties of the surface-bound wave packet, including its carrier wavelength (783 nm) and group velocity (0.95c). In addition, tr-PEEM images reveal that the launched PSP may be detected at least 250 μm away from the coupling trench structure.

Sub-nanosecond signal propagation in anisotropy-engineered nanomagnetic logic chains

Energy efficient nanomagnetic logic (NML) computing architectures propagate binary information by relying on dipolar field coupling to reorient closely spaced nanoscale magnets. Signal propagation in nanomagnet chains has been previously characterized by static magnetic imaging experiments; however, the mechanisms that determine the final state and their reproducibility over millions of cycles in high-speed operation have yet to be experimentally investigated. Here we present a study of NML operation in a high-speed regime. We perform direct imaging of digital signal propagation in permalloy nanomagnet chains with varying degrees of shape-engineered biaxial anisotropy using full-field magnetic X-ray transmission microscopy and time-resolved photoemission electron microscopy after applying nanosecond magnetic field pulses. An intrinsic switching time of 100 ps per magnet is observed. These experiments, and accompanying macrospin and micromagnetic simulations, reveal the underlying physics of NML architectures repetitively operated on nanosecond timescales and identify relevant engineering parameters to optimize performance and reliability.

Nanoscale sub-100 picosecond all-optical magnetization switching in GdFeCo microstructures.

Ultrafast magnetization reversal driven by femtosecond laser pulses has been shown to be a promising way to write information. Seeking to improve the recording density has raised intriguing fundamental questions about the feasibility of combining ultrafast temporal resolution with sub-wavelength spatial resolution for magnetic recording. Here we report on the experimental demonstration of nanoscale sub-100 ps all-optical magnetization switching, providing a path to sub-wavelength magnetic recording. Using computational methods, we reveal the feasibility of nanoscale magnetic switching even for an unfocused laser pulse. This effect is achieved by structuring the sample such that the laser pulse, via both refraction and interference, focuses onto a localized region of the structure, the position of which can be controlled by the structural design. Time-resolved photo-emission electron microscopy studies reveal that nanoscale magnetic switching employing such focusing can be pushed to the sub-100 ps regime.

Time-resolved photoemission electron microscopy imaging of mode coupling between three interacting magnetic vortices

The interactions between three magnetic vortices in a planar equilateral triangular arrangement were studied by time-resolved photoemission electron microscopy. The gyrotropic resonance frequencies of the three individual vortices in the tri-disk system are different from one another and also shifted from that of an isolated vortex by as much as 12%. A comparison with analytical calculations and numerical simulations shows that the observed frequency shifts result from the dipolar interaction between the vortices.

Femtosecond time-resolved photoemission electron microscopy for spatiotemporal imaging of photogenerated carrier dynamics in semiconductors.

We constructed an instrument for time-resolved photoemission electron microscopy (TR-PEEM) utilizing femtosecond (fs) laser pulses to visualize the dynamics of photogenerated electrons in semiconductors on ultrasmall and ultrafast scales. The spatial distribution of the excited electrons and their relaxation and/or recombination processes were imaged by the proposed TR-PEEM method with a spatial resolution about 100 nm and an ultrafast temporal resolution defined by the cross-correlation of the fs laser pulses (240 fs). A direct observation of the dynamical behavior of electrons on higher resistivity samples, such as semiconductors, by TR-PEEM has still been facing difficulties because of space and/or sample charging effects originating from the high photon flux of the ultrashort pulsed laser utilized for the photoemission process. Here, a regenerative amplified fs laser with a widely tunable repetition rate has been utilized, and with careful optimization of laser parameters, such as fluence and repetition rate, and consideration for carrier lifetimes, the electron dynamics in semiconductors were visualized. For demonstrating our newly developed TR-PEEM method, the photogenerated carrier lifetimes around a nanoscale defect on a GaAs surface were observed. The obtained lifetimes were on a sub-picosecond time scale, which is much shorter than the lifetimes of carriers observed in the non-defective surrounding regions. Our findings are consistent with the fact that structural defects induce mid-gap states in the forbidden band, and that the electrons captured in these states promptly relax into the ground state.

The Interplay between Localized and Propagating Plasmonic Excitations Tracked in Space and Time

In this work, the mutual coupling and coherent interaction of propagating and localized surface plasmons within a model-type plasmonic assembly is experimentally demonstrated, imaged, and analyzed. Using interferometric time-resolved photoemission electron microscopy the interplay between ultrashort surface plasmon polariton wave packets and plasmonic nanoantennas is monitored on subfemtosecond time scales. The data reveal real-time insights into dispersion and localization of electromagnetic fields as governed by the elementary modes determining the functionality of plasmonic operation units.

Direct imaging of electron recombination and transport on a semiconductor surface by femtosecond time-resolved photoemission electron microscopy

Much effort has been devoted to the development of techniques to probe carrier dynamics, which govern many semiconductor device characteristics. We report direct imaging of electron dynamics on semiconductor surfaces by time-resolved photoemission electron microscopy using femtosecond laser pulses. The experiments utilized a variable-repetition-rate femtosecond laser system to suppress sample charging problems. The recombination of photogenerated electrons and the lateral motion of the electrons driven by an external electric field on a GaAs surface were visualized. The mobility was estimated from a linear relationship between the drift velocity and the potential gradient.

Dynamics of laser-induced spin reorientation in Co/SmFeO3heterostructure

Ultrafast control of a ferromagnet (FM) via exchange coupling with an antiferromagnet (AFM) is demonstrated in a Co/SmFeO${}_{3}$ heterostructure. Employing time-resolved photoemission electron microscopy combined with x-ray magnetic circular dichroism, a sub-100-ps change of the Co spins orientation by up to 10${}^{\ensuremath{\circ}}$ driven by the ultrafast heating of the SmFeO${}_{3}$ orthoferrite substrate through its spin reorientation phase transition is revealed. Numerical modeling of the ultrafast-laser-induced heat profile in the heterostructure, and the subsequent coupled spins dynamics and equilibration of the spin systems suggest that the localized laser-induced spin reorientation is hindered compared with the static case. Moreover, numerical simulations show that a relatively small Co/SmFeO${}_{3}$ exchange interaction could be sufficient to induce a complete and fast spin reorientation transition (SRT).