Current advances in ultrafast electron microscopy make it possible to combine optical pumping of a nanostructure and electron beam probing with subångstrom and femtosecond spatiotemporal resolution. We present a theory predicting that this technique can reveal a rich out-of-equilibrium dynamics of plasmon excitations in graphene and graphite samples. In a disruptive departure from the traditional probing of nanoscale excitations based on the identification of spectral features in the transmitted electrons, we show that measurement of angle-resolved, energy-integrated inelastic electron scattering can trace the temporal evolution of plasmons in these structures and provide momentum-resolved mode identification, thus avoiding the need for highly-monochromatic electron beams and the use of electron spectrometers. This previously unexplored approach to study the ultrafast dynamics of optical excitations can be of interest to understand and manipulate polaritons in 2D semiconductors and other materials exhibiting a strong thermo-optical response.
We demonstrate that ultrafast carrier excitation can drastically affect electronic structures and induce brief surface plasmonic response in non-plasmonic metals, potentially creating a plasmonic switch. Using first-principles molecular dynamics and Kubo-Greenwood formalism for laser-excited tungsten we show that carrier heating mobilizes d electrons into collective inter and intraband transitions leading to a sign flip in the imaginary optical conductivity, activating plasmonic properties for the initial non-plasmonic phase. The drive for the optical evolution can be visualized as an increasi…
We measure nonlinear optical scattering from individual Au nanorods excited by ultrafast laser pulses on resonance with their longitudinal plasmon mode. Isolating single rods removes inhomogeneous broadening and allows the measurement of a large nonlinearity, much greater than that of nanorod ensembles. Surprisingly, the ultrafast nonlinearity can be attributed entirely to heating of conduction electrons and does not exhibit any response associated with coherent plasmon oscillation. This indicates a previously unobserved damping of strongly driven plasmons.
The dielectric response of transparent conductive oxides near the bulk plasmon frequency is characterized by a refractive index less than vacuum. In analogy with x-ray optics, it is shown that this regime results in total external reflection and air-guiding of light. In addition, the strong reduction of the wavevector in the ITO below that of free space enables a new surface plasmon polariton mode which can be excited without requiring a prism or grating coupler. Ultrafast control of the surface plasmon polariton mode is achieved with a modulation amplitude reaching 20%.
Ultrafast demagnetization in magnetic nanoparticles using pulsed laser has attracted considerable attention because of its potential applications in spintronics, such as data storage. In such applications, it is necessary to control magnetization using low energy laser pulses, however, this poses the problem of increasing the amount of energy from the excitation laser pulses to the spin subsystem. We take advantage of the phenomenon known as localized surface plasmon resonance (LSPR) to enhance the energy transfer from laser pulses to the spin subsystem. To induce LSPR, hybrid nanoparticles co…
Exploring low-loss two-dimensional plasmon modes is considered central for achieving light manipulation at the nanoscale and applications in plasmonic science and technology. In this context, pump-probe spectroscopy is a powerful tool for investigating these collective modes and the corresponding energy transfer processes. Here, I present a first-principles study on non-equilibrium Dirac plasmon in graphene, wherein damping channels under ultrafast conditions are still not fully explored. The laser-induced blueshift of plasmon energy is explained in terms of thermal increase of the electron-ho…
We demonstrate that the dispersion of surface plasmon polaritons in a periodically perforated gold film can be efficiently manipulated by femtosecond laser pulses with the wavelengths far from the intrinsic resonances of gold. Using a time- and frequency- resolved pump-probe technique we observe shifting of the plasmon polariton resonances with response times from 200 to 800 fs depending on the probe photon energy, through which we obtain comprehensive insight into the electron dynamics in gold. We show that Wood anomalies in the optical spectra provide pronounced resonances in differential tr…
Ultrafast plasmonics of novel materials has emerged as a promising field of nanophotonics bringing new concepts for advanced optical applications. Ultrafast electronic photoexcitation of a diamond surface and subsequent surface plasmon-polaritons (SPPs) excitation are studied both theoretically and experimentally - for the first time. After photoexcitation on the rising edge of the pulse, transient surface metallization was found to occur for laser intensity near 18 TW/cm$^2$ due to enhancement of the impact ionization rate; in this regime, the dielectric constant of the photoexcited diamond b…
Electron-hole generation and recombination rates for plasmon emission and absorption in Graphene are presented. The recombination times of carriers due to plasmon emission have been found to be in the tens of femtoseconds to hundreds of picoseconds range. The recombination times depend sensitively on the carrier energy, carrier density, temperature, and the plasmon dispersion. Carriers near the Dirac point are found to have much longer lifetimes compared to carriers at higher energies. Plasmons in a Graphene layer on a polar substrate hybridize with the surface optical phonons and this hybridi…
We report the investigation of the generation and detection of GHz coherent acoustic phonons in plasmonic gold nanoparticles superlattices (NPS). The experiments have been performed from an optical femtosecond pump-probe scheme across the optical plasmon resonance of the superlattice. Our experiments allow to estimate the collective elastic response (sound velocity) of the NPS as well as an estimate of the nano-contact elastic stiffness. It appears that the light-induced coherent acoustic phonon pulse has a typical in-depth spatial extension of about 45 nm which is roughly 4 times the optical …
The nature of a phase transition is inherently connected to the changes in the crystalline symmtry, which is typically probed by elastic or inelastic scattering with neutrons, electrons or photons. When such a phase transition is stimulated by light or other sudden perturbations the solid evolves along a non-equilibrium pathway of which the underlying physics is poorly understood. Here we use picosecond Raman scattering to study the photo-induced ultrafast dynamics in Peierls distorted Antimony. We find evidence for an ultrafast non-thermal reversible structural phase transition. Most surprisi…
Excitation of coherent optical phonons in solids provides a pathway for ultrafast modulation of light on a sub-ps timescale. Here, we report on efficient 3.6 THz modulation of light reflected from hybrid metal/semiconductor plasmonic crystals caused by lattice vibrations in a few nm thick layer of elemental tellurium. We observe that surface plasmon polaritons contribute significantly to photoinduced formation of this thin layer at the interface between a telluride-based II-VI semiconductor, such as (Cd,Mg)Te or (Cd,Mn)Te, and a one-dimensional gold grating. The change in interface composition…
Ultrafast excitation of Bloch plasmon polaritons in hyperbolic metamaterials with an extreme ultra-violet transient grating
Umeå University（于默奥大学）；Elettra Sincrotrone Trieste（的里雅斯特同步辐射中心）；CIC nanoGUNE BRTA（nanoGUNE研究中心）；Ikerbasque, Basque Foundation for Science（伊卡巴斯克，巴斯克科学基金会）；Università degli Studi di Modena e Reggio Emilia（摩德纳和雷焦艾米利亚大学）；Wallenberg Initiative Materials Science for Sustainability（瓦伦堡可持续材料科学倡议）
Recently, van der Waals heterostructure has attracted interest both theoretically and experimentally for their potential applications in photoelectronic devices, photovoltaic devices, plasmonic devices and photocatalysis. Inspired by this, we design a lepidocrocite-type TiO2/GaSe heterostructure. Via first-principles simulations, we show that such a heterostructure is a direct bandgap semiconductor with a strong and broad optical absorption, ranging from visible light to UV region, exhibiting its potential application in photoelectronic and photovoltaic devices. With the planar-averaged electr…
We generate in-plane magnetoelastic waves in nickel films using the all-optical transient grating technique. When performed on amorphous glass substrates, two dominant magnetoelastic excitations can be resonantly driven by the underlying elastic distortions, the Rayleigh Surface Acoustic Wave and the Surface Skimming Longitudinal Wave. An applied field, oriented in the sample plane, selectively tunes the coupling between magnetic precession and one of the elastic waves, thus demonstrating selective excitation of coexisting, large amplitude magnetoelastic waves. Analytical calculations based on…
Topological insulators with their topological protected surface states are highly promising quantum materials. In this article the micro-flakes of single-crystalline topological insulators Bi2Te3 and Sb2Te3 are explored through physical parameter measurement at low temperatures and thereby the charge carrier dynamics are investigated at 5K to study the various optical transitions related to these surface states. The magnetoresistance is experimentally investigated at temperatures of 5K and 100K for a field range of 1Tesla. The occurrence of the weak anti-localization effect predicts the presen…
Dirac plasmons in graphene are very sensitive to the dielectric properties of the environment. We show that this can be used to probe the structure and composition of van der Waals heterostructures (vdWh) put underneath a single graphene layer. In order to do so, we assess vdWh composed of hexagonal boron nitride and different types of transition metal dichalcogenides (TMDs). By performing realistic simulations that account for the contribution of each layer of the vdWh separately and including the importance of the substrate phonons, we show that one can achieve single-layer resolution by inv…
Hybrid plasmonic photonic structures combine the plasmonic response with the photonic band gap, holding promise for utilization as optical switches and sensors. Here, we demonstrate the active modulation of the optical response in such structures with two different external stimuli, e.g. laser pulses and bacteria. First, we report the fabrication of a miniaturized (5 x 5 mm) indium tin oxide (ITO) grating employing femtosecond laser micromachining, and we show the possibility to modulate the photonic band gap in the visible via ultrafast photoexcitation in the infrared part of the spectrum. No…
It has been technically challenging to concurrently probe the electrons and the lattices in materials during non-equilibrium processes, allowing their correlations to be determined. Here, in a single set of ultrafast electron diffraction patterns taken on the charge-density-wave (CDW) material 1T-TaSeTe, we discover a temporal shift in the diffraction intensity measurements as a function of scattering angle. With the help of dynamic models and theoretical calculations, we show that the ultrafast electrons probe both the valence-electron and lattice dynamic processes, resulting in the temporal …
We report an ultrafast electron diffraction study of silver nanocrystals under surface plasmon resonance excitation, leading to a concerted fragmentation. By examining simultaneously transient structural, thermal, and Coulombic signatures of the prefragmented state, an electronically driven nonthermal fragmentation scenario is proposed.
High-quality emission centers in two-dimensional materials are promising components for future photonic and optoelectronic applications. Carbon-enriched hexagonal boron nitride (hBN:C) layers host atom-like color-center (CC) defects with strong and robust photoemission up to room temperature. Placing the hBN:C layers on top of Ag triangle nanoparticles (NPs) accelerate the decay of the CC defects down to 46 ps from their reference bulk value of 350 ps. The ultrafast decay is achieved due to the efficient excitation of the plasmon modes of the Ag NPs by the near field of the CCs. Simulations of…
Trisoctahedral (TOH) shaped Au nanocrystals (NCs) have emerged as a new class of metal nanoparticles (MNP) due to its superior catalystic and SERS activities caused by the presence of high density atomic steps and dangling bonds on their high index facets. We examine the radiative localized surface plasmon resonance (LSPR) modes of an isolated single TOH Au NC using cathodoluminescence (CL), with high resolution spatial information of the local density of optical states (LDOS) across the visible spectral range. Further we show pronounced enhancement factor in the Raman scattering by performing…
We uncovered for the first time the spin dynamics involved in the birth and growth of giant spin polarons in a magnetic semiconductor. For this purpose, we developed a new measurement technique, which for the first time provides direct access to the spin dynamics, irrespective of phonons and carriers involved in the process. Moreover, we solved for the first time the Landau-Liftshitz equation in the specific scenario of spin polarons, which fits our data excellently, and demonstrates for the first time that the spin polaron growth slows down dramatically when the sample is cooled in the parama…
Probing Plasmonic Oscillations in 2D Moiré Nanocrystal Superlattices by Low-Loss EELS
University of Pennsylvania（宾夕法尼亚大学）；University of Washington（华盛顿大学）；SuperSTEM, SciTech Daresbury Science and Innovation Campus（超级扫描透射电子显微镜，科学技术达尔斯伯里科学与创新园区）；University of Leeds（利兹大学）
We present a theoretical investigation of the yet unexplored ultrafast processes and dynamics of the produced excited carriers upon irradiation of Silicon with femtosecond pulsed lasers in the mid-infrared (mid-IR) spectral region. The evolution of the carrier density and thermal response of the electron-hole and lattice subsystems are analysed for various wavelengths λL in the range between 2.2 μm and 3.3 μm where the influence of two and three-photon absorption mechanisms is explored. The role of induced Kerr effect is highlighted and it manifests a more pronounced influence at smaller wavel…
Recently, the switching between the different charge-ordered phases of 1T-TaS2 has been probed by ultrafast techniques, revealing unexpected phenomena such as "hidden" metastable states and peculiar photoexcited charge patterns. Here, we apply broadband pump-probe spectroscopy with varying excitation energy to study the ultrafast optical properties of 1T-TaS2 in the visible regime. By scanning the excitation energy in the near-IR region we unravel the coupling between different charge excitations and the low-lying charge-density wave state. We find that the amplitude mode of the charge-density…
We present a flexible and efficient ultrafast time-resolved spontaneous Raman spectroscopy setup to study collective excitation and quasi-particle dynamics in quantum matter. The setup has a broad energy tuning range extending from the visible to near infrared spectral regions for both the pump excitation and Raman probe pulses. Additionally, the balance between energy and time-resolution can be controlled. A high light collecting efficiency is realized by high numerical aperture collection optics and a high-throughput flexible spectrometer. We demonstrate the functionality of the setup with a…
Fundamental interactions induced by lattice vibrations on ultrafast time scales become increasingly important for modern nanoscience and technology. Experimental access to the physical properties of acoustic phonons in the THz frequency range and over the entire Brillouin zone is crucial for understanding electric and thermal transport in solids and their compounds. Here, we report on the generation and nonlinear propagation of giant (1 percent) acoustic strain pulses in hybrid gold/cobalt bilayer structures probed with ultrafast surface plasmon interferometry. This new technique allows for un…
Plasmonics, the science and technology of the interaction of light with metallic objects, is fundamentally changing the way we can detect, generate and manipulate light. Although the field is progressing swiftly, thanks to the availability of nanoscale manufacturing and analysis methods, fundamental properties such as the plasmonic excitations' symmetries cannot be accessed directly, leading to a partial, sometimes incorrect, understanding of their properties. Here we overcome this limitation by deliberately shaping the wave function of an electron beam to match a plasmonic excitations' symmet…
Ultrafast optical pulses are an increasingly important tool for controlling quantum materials and triggering novel photo-induced phase transitions. Understanding these dynamic phenomena requires a probe sensitive to spin, charge, and orbital degrees of freedom. Time-resolved resonant inelastic X-ray scattering (trRIXS) is an emerging spectroscopic method, which responds to this need by providing unprecedented access to the finite-momentum fluctuation spectrum of photoexcited solids. In this Perspective, we briefly review state-of-the-art trRIXS experiments on condensed matter systems, as well …
In this paper we analyze the effects of nonlocality on the optical properties of a system consisting of a thin metallic film separated from a graphene sheet by a hexagonal boron nitride (hBN) layer. We show that nonlocal effects in the metal have a strong impact on the spectrum of the surface plasmon-polaritons on graphene. If the graphene sheet is shaped into a grating, we show that the extinction curves can be used to shed light on the importance of nonlocal effects in metals. Therefore, graphene surface plasmons emerge as a tool for probing nonlocal effects in metallic nanostructures, inclu…
The control of optically driven high-frequency strain waves in nanostructured systems is an essential ingredient for the further development of nanophononics. However, broadly applicable experimental means to quantitatively map such structural distortion on their intrinsic ultrafast time and nanometer length scales are still lacking. Here, we introduce ultrafast convergent beam electron diffraction (U-CBED) with a nanoscale probe beam for the quantitative retrieval of the time-dependent local distortion tensor. We demonstrate its capabilities by investigating the ultrafast acoustic deformation…
Ultrafast THz radiation generation from ferromagnetic/nonmagnetic bilayer heterostructure-based spintronic emitters generally exploits the conversion from spin- to charge-current within the nonmagnetic layer and its interface with the ferromagnetic layer. Various possible sub-contributions to the underlying mechanism of inverse spin Hall effect for the THz emission from such structures, need to be exploited for not only investigating the intricacies at the fundamental level in the material properties themselves but also for improving their performance for broadband and high-power THz emission.…
A periodic arrangement of 2D conducting planes is known to host a (bulk) plasmon dispersion that interpolates between the typical, gapped behavior of 3D metals and a gapless, acoustic regime as a function of the out-of-plane wavevector. The semi-infinite system -- the configuration relevant to Electron Energy Loss Spectroscopy (EELS) in a reflection geometry, as in High Resolution EELS (HREELS) -- is known to host a surface plasmon that ceases to propagate below a cutoff wavevector. As the f-sum rule requires a finite response whether or not there exist sharp excitations, we demonstrate that w…
Metal-corroles are macrocycle organic molecules with numerous practical applications. In particular, copper corroles exhibit an interesting saddled geometry, which has attracted significant attention from theoreticians and experimentalists over the years. The present work is dedicated to understand the effect of structural saddling in a copper corrole on potential probe signals via imaging ultrafast coherent electron dynamics. A linearly polarized pulse is used to trigger the electron dynamics and time-resolved x-ray diffraction is employed to image the triggered dynamics. It is found that the…
Optical control of electronic spins is the basis for ultrafast spintronics: circularly polarized light in combination with spin-orbit coupling of the electronic states allows for spin manipulation in condensed matter. However, the conventional approach is limited to spin orientation along one particular orientation that is dictated by the direction of photon propagation. Plasmonics opens new capabilities, allowing one to tailor the light polarization at the nanoscale. Here, we demonstrate ultrafast optical excitation of electron spin on femtosecond time scales via plasmon to exciton spin conve…
We investigate the relaxation dynamics of photogenerated carriers in silicon nanowires consisting of a crystalline core and a surrounding amorphous shell, using femtosecond time-resolved differential reflectivity and transmission spectroscopy at photon energies of 3.15 eV and 1.57 eV. The complex behavior of the differential transmission and reflectivity transients is the mixed contributions from the crystalline core and the amorphous silicon on the nanowire surface and the substrate where competing effects of state filling and photoinduced absorption govern the carrier dynamics. Faster relaxa…
Excitons and plasmons are the two most fundamental types of collective electronic excitations occurring in solids. Traditionally, they have been studied separately using bulk techniques that probe their average energetic structure over large spatial regions. However, as the dimensions of materials and devices continue to shrink, it becomes crucial to understand how these excitations depend on local variations in the crystal- and chemical structure on the atomic scale. Here we use monochromated low-loss scanning-transmission-electron-microscopy electron-energy-loss (LL-STEM-EEL) spectroscopy, p…
Disentangling the primary order parameter from secondary order parameters in phase transitions is critical to the interpretation of the transition mechanisms in strongly correlated systems and quantum materials. Here we present a study of structural phase transition pathways in superionic Cu2S nanocrystals that exhibit intriguing properties. Utilizing ultrafast electron diffraction techniques sensitive in both momentum-space and the time-domain, we distinguish the dynamics of crystal symmetry breaking and lattice expansion in this system. We are able to follow the transient states along the tr…
Ultrafast laser measurements probe the non-equilibrium dynamics of excited electrons in metals with increasing temporal resolution. Electronic structure calculations can provide a detailed microscopic understanding of hot electron dynamics, but a parameter-free description of pump-probe measurements has not yet been possible, despite intensive research, because of the phenomenological treatment of electron-phonon interactions. We present ab initio predictions of the electron-temperature dependent heat capacities and electron-phonon coupling coefficients of plasmonic metals. We find substantial…
SmB6 is a promising candidate for topological Kondo insulator. In this letter, we report ultrafast carrier dynamics of SmB6. Two characteristic temperatures: T1=100 K and T2= 20 K are observed. T1 corresponds to the opening of the f-d hybridization gap revealed by an abrupt disappearance of terahertz f-band plasmon oscillations. Between T1 and T2, a phonon bottleneck effect dominates the photocarrier relaxation processes. Below T2, we observe the formation of in-gap states, which are strongly affected by optically injected hot electrons and the transient electron temperature change.
