Time-resolved Photoemission Electron Microscopy Research Articles

Lifetime mapping using femtosecond time-resolved photoemission electron microscopy.

Time-resolved photoemission electron microscopy (PEEM) has established itself as a versatile experimental technique to unravel the ultrafast electron dynamics of materials with nanometer-scale resolution. However, the approach of performing PEEM-based, pixel-by-pixel lifetime mapping has not been reported thus far. Herein, we describe in detail the data pre-processing procedure and an algorithm to perform time-trace fittings of each pixel. We impose an energy cutoff for each pixel prior to spectral integration to enhance the robustness of our approach. With the energy cutoff, the energy-integrated time traces show improved statistics and lower fitting errors, thus resulting in a more accurate determination of the fit parameters, e.g., decay time constants. Our work allows us to reliably construct PEEM-based lifetime maps, which potentially shed light on the effects of local microenvironment on the ultrafast processes of the material and allow spatial distributions of lifetimes to be correlated with observables obtained from complementary microscopic techniques, hence enabling a more comprehensive characterization of the material.

Acoustic phonon excitation in gold probed by time-resolved photoemission electron microscopy.

Electron-phonon coupling is an important energy transfer mechanism in solids after ultrafast laser excitation. In this study, we present an extreme ultraviolet (EUV) and infrared (IR) pump-probe photoemission experiment to investigate the electron-phonon coupling in nonequilibrium gold. The energy of IR-laser-emitted photoelectrons is shifted due to the EUV photoemission and oscillates with a ∼4THz frequency. Such oscillation is considered as the effective excitation of the longitudinal acoustic phonon mode in gold through the spectral-dependent electron-phonon coupling. Our study showcases the capability of time-resolved photoemission electron microscopy to monitor the non-equilibrium lattice vibrations with ultrahigh spatial and temporal resolution.

Momentum space separation of quantum path interferences between photons and surface plasmon polaritons in nonlinear photoemission microscopy

Abstract Quantum path interferences occur whenever multiple equivalent and coherent transitions result in a common final state. Such interferences strongly modify the probability of a particle to be found in that final state, a key concept of quantum coherent control. When multiple nonlinear and energy-degenerate transitions occur in a system, the multitude of possible quantum path interferences is hard to disentangle experimentally. Here, we analyze quantum path interferences during the nonlinear emission of electrons from hybrid plasmonic and photonic fields using time-resolved photoemission electron microscopy. We experimentally distinguish quantum path interferences by exploiting the momentum difference between photons and plasmons and through balancing the relative contributions of their respective fields. Our work provides a fundamental understanding of the nonlinear photon–plasmon–electron interaction. Distinguishing emission processes in momentum space, as introduced here, could allow nano-optical quantum-correlations to be studied without destroying the quantum path interferences.

Ultrafast Charge Transfer and Recombination Dynamics in Monolayer-Multilayer WSe2 Junctions Revealed by Time-Resolved Photoemission Electron Microscopy.

The ultrafast carrier dynamics of junctions between two chemically identical, but electronically distinct, transition metal dichalcogenides (TMDs) remains largely unknown. Here, we employ time-resolved photoemission electron microscopy (TR-PEEM) to probe the ultrafast carrier dynamics of a monolayer-to-multilayer (1L-ML) WSe2 junction. The TR-PEEM signals recorded for the individual components of the junction reveal the sub-ps carrier cooling dynamics of 1L- and 7L-WSe2, as well as few-ps exciton-exciton annihilation occurring on 1L-WSe2. We observe ultrafast interfacial hole (h) transfer from 1L- to 7L-WSe2 on an ∼0.2 ps time scale. The resultant excess h density in 7L-WSe2 decays by carrier recombination across the junction interface on an ∼100 ps time scale. Reminiscent of the behavior at a depletion region, the TR-PEEM image reveals the h density accumulation on the 7L-WSe2 interface, with a decay length ∼0.60 ± 0.17 μm. These charge transfer and recombination dynamics are in agreement with ab initio quantum dynamics. The computed orbital densities reveal that charge transfer occurs from the basal plane, which extends over both 1L and ML regions, to the upper plane localized on the ML region. This mode of charge transfer is distinctive to chemically homogeneous junctions of layered materials and constitutes an additional carrier deactivation pathway that should be considered in studies of 1L-TMDs found alongside their ML, a common occurrence in exfoliated samples.

Ultrafast Time Dynamics of Plasmonic Fractional Orbital Angular Momentum.

The creation and manipulation of optical vortices, both in free space and in two-dimensional systems such as surface plasmon polaritons (SPPs), has attracted widespread attention in nano-optics due to their robust topological structure. Coupled with strong spatial confinement in the case of SPPs, these plasmonic vortices and their underlying orbital angular momentum (OAM) have promise in novel light-matter interactions on the nanoscale with applications ranging from on-chip particle manipulation to tailored control of plasmonic quasiparticles. Until now, predominantly integer OAM values have been investigated. Here, we measure and analyze the time evolution of fractional OAM SPPs using time-resolved two-photon photoemission electron microscopy and near-field optical microscopy. We experimentally show the field's complex rotational dynamics and observe the beating of integer OAM eigenmodes at fractional OAM excitations. With our ability to access the ultrafast time dynamics of the electric field, we can follow the buildup of the plasmonic fractional OAM during the interference of the converging surface plasmons. By adiabatically increasing the phase discontinuity at the excitation boundary, we track the total OAM, leading to plateaus around integer OAM values that arise from the interplay between intrinsic and extrinsic OAM.

Ultrafast Electronic Dynamics in Anisotropic Indirect Interlayer Excitonic States of Monolayer WSe2/ReS2 Heterojunctions.

Understanding ultrafast electronic dynamics of the interlayer excitonic states in atomically thin transition metal dichalcogenides is of importance in engineering valleytronics and developing excitonic integrated circuits. In this work, we experimentally explored the ultrafast dynamics of indirect interlayer excitonic states in monolayer type II WSe2/ReS2 heterojunctions using time-resolved photoemission electron microscopy, which reveals its anisotropic behavior. The ultrafast cooling and decay of excited-state electrons exhibit significant linear dichroism. The ab initio theoretical calculations provide unambiguous evidence that this linear dichroism result is primarily associated with the anisotropic nonradiative recombination of indirect interlayer excitonic states. Measuring time-resolved photoemission energy spectra, we have further revealed the ultrafast evolution of excited-state electrons in anisotropic indirect interlayer excitonic states. The findings have important implications for controlling the interlayer moiré excitonic effects and designing anisotropic optoelectronic devices.

Ultrafast Electronic Relaxation Dynamics of Atomically Thin MoS2 Is Accelerated by Wrinkling.

Strain engineering is an attractive approach for tuning the local optoelectronic properties of transition metal dichalcogenides (TMDs). While strain has been shown to affect the nanosecond carrier recombination dynamics of TMDs, its influence on the sub-picosecond electronic relaxation dynamics is still unexplored. Here, we employ a combination of time-resolved photoemission electron microscopy (TR-PEEM) and nonadiabatic ab initio molecular dynamics (NAMD) to investigate the ultrafast dynamics of wrinkled multilayer (ML) MoS2 comprising 17 layers. Following 2.41 eV photoexcitation, electronic relaxation at the Γ valley occurs with a time constant of 97 ± 2 fs for wrinkled ML-MoS2 and 120 ± 2 fs for flat ML-MoS2. NAMD shows that wrinkling permits larger amplitude motions of MoS2 layers, relaxes electron-phonon coupling selection rules, perturbs chemical bonding, and increases the electronic density of states. As a result, the nonadiabatic coupling grows and electronic relaxation becomes faster compared to flat ML-MoS2. Our study suggests that the sub-picosecond electronic relaxation dynamics of TMDs is amenable to strain engineering and that applications which require long-lived hot carriers, such as hot-electron-driven light harvesting and photocatalysis, should employ wrinkle-free TMDs.

Revealing low-loss dielectric near-field modes of hexagonal boron nitride by photoemission electron microscopy

Low-loss dielectric modes are important features and functional bases of fundamental optical components in on-chip optical devices. However, dielectric near-field modes are challenging to reveal with high spatiotemporal resolution and fast direct imaging. Herein, we present a method to address this issue by applying time-resolved photoemission electron microscopy to a low-dimensional wide-bandgap semiconductor, hexagonal boron nitride (hBN). Taking a low-loss dielectric planar waveguide as a fundamental structure, static vector near-field vortices with different topological charges and the spatiotemporal evolution of waveguide modes are directly revealed. With the lowest-order vortex structure, strong nanofocusing in real space is realized, while near-vertical photoemission in momentum space and narrow spread in energy space are simultaneously observed due to the atomically flat surface of hBN and the small photoemission horizon set by the limited photon energies. Our approach provides a strategy for the realization of flat photoemission emitters.

High spatiotemporal resolved imaging of ultrafast control of nondiffracting surface plasmon polaritons

Abstract Nondiffracting Bessel surface plasmon polariton (SPP) beams, which have unique self-healing, non-divergence, and linear transmission properties, have charming applications in plasmonic devices and on-chip interconnection circuits. Here we first realize, to the best of our knowledge, the ultrafast control and imaging of the Bessel SPP pulse on the nano-femto scale in the experiment. We demonstrate ultrafast control of Bessel SPP pulse switching by controlling the instantaneous polarization state of the excitation light. Moreover, this variation process is directly mapped on the nano-femto scale by time-resolved two-color photoemission electron microscopy. The results are well reproduced by the finite-difference time-domain (FDTD) method. The current study of ultrafast control and spatiotemporally imaging the switching process establishes an experimental paradigm for revealing the complex mechanisms in ultrafast control of nondiffracting SPP and are useful for developing high-speed, highly-integrated nanophotonic devices, and on-chip circuits.

Development of in situ characterization of two-dimensional materials grown on insulator substrates with spectroscopic photoemission and low energy electron microscopy

Ultrathin two-dimensional (2D) materials offer great potential for next-generation integrated circuit and optoelectronic devices. Chemical vapor deposition (CVD)-grown 2D materials provide a way to mass production in industry. However, how to in situ characterize their intrinsic electric/photoelectric properties and carrier dynamics with electron/photoelectron probes is still a problem due to the interference from the conducting substrate. Here, we present a grounding Au grids method to realize in situ characterization of the CVD-grown MoS2 on the insulating thick SiO2 layer covered Si substrate with spectroscopic photoemission and low energy electron microscopy (SPELEEM). Through depositing Au grids afterwards, we have achieved good grounding of MoS2 flakes in the photoemission electron microscopy (PEEM), mirror electron microscopy (MEM), and micro-area low energy electron diffraction (µ-LEED) measurements. We have clarified the false signal caused by stray photoelectrons originated from the Au stripes, and as well as the space charge effects induced by intense photoemission. We have also confirmed that time-resolved PEEM results are not affected by the stray signal, and by adopting a small light spot, both static and time-resolved micro-area photoelectron spectroscopy (µ-PES) can be unaffected by space charge effects. Our results provide a reliable way to in situ investigate 2D materials grown on insulating substrates by probing photoelectrons or backscattered electrons.

Coaction effect of radiative and non-radiative damping on the lifetime of localized surface plasmon modes in individual gold nanorods.

Revealing the coaction effect of radiative and non-radiative damping on the lifetime of the localized surface plasmon resonance (LSPR) mode is a prerequisite for the applications of LSPR. Here, we systematically investigated the coaction effect of radiative and non-radiative damping on the lifetime of the super-radiant and sub-radiant LSPR modes of gold nanorods using time-resolved photoemission electron microscopy (TR-PEEM). The results show that the lifetime of the LSPR mode depends on the length of the gold nanorod, and the different variation behavior of an LSPR mode lifetime exists between the super-radiative mode and the sub-radiative one with the increase of nanorod length (volume). Surprisingly, it is found that the lifetime of the super-radiant LSPR mode can be comparable to or even longer than that of the sub-radiant LSPR mode, instead of the usual claim that a sub-radiant LSPR mode has a longer life than the super-radiant mode. Those TR-PEEM experimental results are supported by finite-difference time-domain simulations and are well explained by the coaction effect with the calculation of the radiative and non-radiative damping rate with the increase of the nanorod volume. We believe that this study is beneficial to build a low-threshold nano-laser and ultrasensitive molecular spectroscopy system.

Flexible manipulation of plasmon dephasing time via the adjustable Fano asymmetric dimer

It is highly desirable to flexibly and actively manipulate the dephasing time of a plasmon in many potential applications; however, this remains a challenge. In this work, by using femtosecond time-resolved photoemission electron microscopy, we experimentally demonstrated that the Fano resonance mode in the asymmetric nanorod dimer can greatly extend the dephasing time of a femtosecond plasmon, whereas the non-Fano resonance results in a smaller dephasing time due to the large radiative damping, and flexible manipulation of the dephasing time can be realized by adjusting one of the nanorods in the Fano asymmetric dimer. Interestingly, it was found that plasmon resonance wavelengths both appeared red-shifted as the length of the upper or lower nanorods increased individually, but the dephasing time varied. Furthermore, it also indicated that the dephasing time can be prolonged with a smaller ascending rate by increasing the length of both the nanorods simultaneously while keeping the dimer asymmetry. Meanwhile, the roles of radiative and nonradiative damping in dephasing time are unveiled in the process of nanorod length variation. These results are well supported by numerical simulations and calculations.

Two-color laser PEEM imaging of horizontal and vertical components of femtosecond surface plasmon polaritons

Explicit visualization of different components of surface plasmon polaritons (SPPs) propagating at dielectric/metal interfaces is crucial in offering chances for the detailed design and control of the functionalities of plasmonic nanodevices in the future. Here, we reported independent imaging of the vertical and horizontal components of SPPs launched from a rectangular trench in the gold film by a 400-nm laser-assisted near-infrared (NIR) femtosecond laser time-resolved photoemission electron microscopy (TR-PEEM). The experiments demonstrate that distinct imaging of different components of SPPs field can be easily achieved by introducing the 400-nm laser. It can circumvent the risk of sample damage and information loss of excited SPPs field that is generally confronted in the usual NIR laser TR-PEEM scheme. The underlying mechanism for realizing distinct imaging of different components of the SPPs field with two-color PEEM is revealed via measuring the double logarithmic dependence of photoemission yield with the 800-nm and 400-nm pulse powers of different polarizations. Moreover, it is found that the PEEM image quality of the vertical and horizontal components of the SPPs field is nearly independent of the 400-nm pulse polarization. These results pave a way for SPPs-based applications and offer a possible solution for drawing a space–time field of SPPs in three dimensions.

Spatiotemporal imaging of the longitudinal and transverse components of the few-cycle surface plasmon polaritons near-field in nano-femto scale by time-resolved photoemission electron microscopy

Spatiotemporal imaging of the longitudinal and transverse components of the few-cycle surface plasmon polaritons near-field in nano-femto scale by time-resolved photoemission electron microscopy

Ultrafast microscopy of a twisted plasmonic spin skyrmion

We report a transient plasmonic spin skyrmion topological quasiparticle within surface plasmon polariton vortices, which is described by analytical modeling and imaging of its formation by ultrafast interferometric time-resolved photoemission electron microscopy. Our model finds a twisted skyrmion spin texture on the vacuum side of a metal/vacuum interface and its integral opposite counterpart in the metal side. The skyrmion pair forming a hedgehog texture is associated with co-gyrating anti-parallel electric and magnetic fields, which form intense pseudoscalar E·B focus that breaks the local time-reversal symmetry and can drive magnetoelectric responses of interest to the axion physics. Through nonlinear two-photon photoemission, we record attosecond precision images of the plasmonic vectorial vortex field evolution with nanometer spatial and femtosecond temporal (nanofemto) resolution, from which we derive the twisted plasmonic spin skyrmion topological textures, their boundary, and topological charges; the modeling and experimental measurements establish a quantized integer photonic topological charge that is stable over the optical generation pulse envelope.

A topological lattice of plasmonic merons

Topology is an intrinsic property of the orbital symmetry and elemental spin–orbit interaction, but also, intriguingly, designed vectorial optical fields can break existing symmetries, to impose (dress) topology through coherent interactions with trivial materials. Through photonic spin–orbit interaction, light can transiently turn on topological interactions, such as chiral chemistry, or induce non-Abelian physics in matter. Employing electromagnetic simulations and ultrafast, time-resolved photoemission electron microscopy, we describe the geometric transformation of a normally incident plane wave circularly polarized light carrying a defined spin into surface plasmon polariton field carrying orbital angular momentum which converges into an array of plasmonic vortices with defined spin textures. Numerical simulations show how within each vortex domain, the photonic spin–orbit interaction molds the plasmonic orbital angular momentum into quantum chiral spin angular momentum textures resembling those of a magnetic meron quasiparticles. We experimentally examine the dynamics of such meron plasmonic spin texture lattice by recording the ultrafast nanofemto plasmonic field evolution with deep subwavelength resolution and sub-optical cycle time accuracy from which we extract the linear polarization, L-line singularity distribution, that defines the periodic lattice boundaries. Our results reveal how vectorial optical fields can impress their topologically nontrivial spin textures by coherent dressing or chiral excitations of matter.

Phyllotaxis-inspired nanosieves with multiplexed orbital angular momentum

Nanophotonic platforms such as metasurfaces, achieving arbitrary phase profiles within ultrathin thickness, emerge as miniaturized, ultracompact and kaleidoscopic optical vortex generators. However, it is often required to segment or interleave independent sub-array metasurfaces to multiplex optical vortices in a single nano-device, which in turn affects the device’s compactness and channel capacity. Here, inspired by phyllotaxis patterns in pine cones and sunflowers, we theoretically prove and experimentally report that multiple optical vortices can be produced in a single compact phyllotaxis nanosieve, both in free space and on a chip, where one meta-atom may contribute to many vortices simultaneously. The time-resolved dynamics of on-chip interference wavefronts between multiple plasmonic vortices was revealed by ultrafast time-resolved photoemission electron microscopy. Our nature-inspired optical vortex generator would facilitate various vortex-related optical applications, including structured wavefront shaping, free-space and plasmonic vortices, and high-capacity information metaphotonics.

Spatially heterogeneous ultrafast interfacial carrier dynamics of 2D-MoS2 flakes

Understanding the ultrafast carrier dynamics of transition metal dichalcogenides is critical for future applications in high-speed electronic and optoelectronic devices. In this work, we used a combination of femtosecond (fs) time-resolved micro-area photoelectron spectroscopy and photoemission electron microscopy (PEEM) to obtain the space-resolved surface photovoltage (SPV) and photoelectron intensity dynamics of two-dimensional (2D) molybdenum disulfide (MoS2) flakes, both of which exhibited high spatial heterogeneity and defect effects. Additionally, surface S vacancy defects were characterized by spatially resolved X-ray photoelectron spectroscopy. The SPV relaxation dynamics indicated that the charge carrier lifetime in the space-charge layer (SCL) ranged from several to tens of nanoseconds and was dominated by the thermionic emission process. The defects, which acted as electron-hole recombination centers, greatly shortened the charge carrier lifetime by almost one order of magnitude. Furthermore, three relaxation processes were observed in the photoelectron intensity dynamics, namely, two fast processes with rates of 3–6 ps (ps) and 60–100 ps, which were largely affected by the defect density, and one slow relaxation process with a rate of 2–5 ns (ns). However, these were not related to the defect density and were attributed to the transportation of electrons towards the bulk. Therefore, our results provide a deeper understanding of the interfacial carrier dynamics of 2D-MoS2 materials and the effects of defects on charge carrier lifetime in the SCL.

Plasmonic vortex cavities multiply OAM

Nanooptics Orbital angular momentum (OAM) of light can be confined to metal surfaces in the form of plasmonic vortices, where nanoscale twisted light oscillates together with the free electrons in metal. Spektor et al. introduced the reflection from structural boundaries as a new degree of freedom to generate and control this surface-confined angular momentum. They designed vortex cavities with chiral boundaries, in which subsequent reflections increased the vortex OAM by multiples of the chiral cavity order. They then tracked the spatiotemporal dynamics of the plasmon pulse trains within the vortex cavities using time-resolved photoemission electron microscopy with sub-femtosecond resolution. These results may have applications in quantum initialization schemes and potentially achieve vortex lattice cavities with dynamically evolving topology. Sci.Adv. 10.1126/sciadv.abg5571 (2021).

Revealing the Chiroptical Response of Plasmonic Nanostructures at the Nanofemto Scale.

The spatiotemporal origin of plasmonic chiroptical responses in nanostructures remains unexplored and unclear. Here, two orthogonally oriented Au nanorods as a prototype were investigated, with a giant chiroptical response caused by antisymmetric and symmetric mode excitations for obliquely incident left-handed circular polarization (LCP) and right-handed circular polarization (RCP) light. Time-resolved photoemission electron microscopy (PEEM) was employed to measure the near-field spatial distributions, spectra, and spatiotemporal dynamics of plasmonic modes associated with the chiroptical responses at the nanofemto scale, verifying the characteristic near-field distributions at the resonant wavelengths of the two modes and a very large spectral dichroism for LCP and RCP. More importantly, eigenmode excitations and their contributions to the ultrafast plasmonic chiroptical response in the space-time domain were directly revealed, promoting a full understanding of the ultrafast chiral origin in complex nanostructures. These findings open a way to design chiroptical nanophotonic devices for spatiotemporal control of chiral light-matter interactions.