Plasmon Polariton Wave Packets Research Articles

Patterning of transition metal dichalcogenides catalyzed by surface plasmons with atomic precision

Summary Plasmon-induced charge transfer has drawn considerable interests and spurred rapid developments of photovoltaics and photocatalysis. Various plasmonic metal/transition metal dichalcogenide (TMD) heterostructures have been developed to promote charge separation. For plasmon-induced catalysis, the transformation of TMDs is rare, and the erosion of TMDs has not yet been reported. Here, we report the etching of two-dimensional TMDs by planar surface plasmon polaritons (SPPs). We found that SPPs can etch various TMDs into desired layers and lateral size through controlling the light power and incident direction. In aqueous media, the strong plasmonic coupling at Au/MoS2 interface generates holes in the valence band of MoS2 that can weaken its interlayer interaction. As a synergistic effect, the plasmonic hot electrons produce oxidizing H2O2 to dissolve MoS2 from the top layers. Our results provide a new perspective for understanding the plasmonic coupling at metal-TMD interfaces and a reliable route toward fabricating well-defined TMDs.

Direct Observation of Surface Plasmon Polariton Propagation and Interference by Time-Resolved Imaging in Normal-Incidence Two Photon Photoemission Microscopy

Time-resolved imaging of the propagation and interference of isolated ultrashort surface plasmon polariton wave packets is demonstrated using two photon photoemission microscopy. The group- and phase velocity of individual wave packets are determined experimentally. Using two counter-propagating surface plasmon polariton pulses, the transient formation of a standing surface plasmon polariton wave is imaged in time and space. We demonstrate that using a normal incidence geometry in time-resolved photoemission microscopy provides great advantages for in-situ imaging of surface plasmon polaritons in arbitrary plasmonic structures. A simple 1D wave-simulation is used to confirm the experimental results.

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.

Focusing surface plasmon polariton wave packets in space and time

AbstractThe spatiotemporal focusing of surface plasmon polariton (SPP) wave packets (WPs) by planar plasmonic‐lens coupling structures is described using combined femtosecond interferometric time‐resolved photoemission electron microscopy (ITR‐PEEM) imaging and model simulations. The focusing properties of lens structures inscribed lithographically into Ag films depend on the angle of incidence of the excitation field. Severe aberrations are introduced by the phase delay in the interaction of obliquely incident plane waves with the commonly employed circular arc‐shaped lens structures. It is shown that the aberration can be corrected by accounting for propagation delays caused by the incidence angle‐dependent retardation of the optical field‐lens structure interaction. The focusing of SPP‐WPs in both space and time is demonstrated with aberration corrected lens structures.

On Plasmon Polariton Propagation Along Metallic Nano-Chain

The collective wave type plasmon polariton self–modes in the metallic (Au, Ag) nano-chain were determined and analyzed with respect to the nano-sphere size and chain separation parameters. At some regions for parameters, the undamped modes were identified when the interaction had been assumed as the near-field-zone dipole coupling. These modes were found on the rim of stability of the linear theory, which indicates artifact of the model of near-field coupling. Inclusion of the medium- and far-field zone contributions to dipole interaction removes, however, instability and allows for fully analytical demonstration of quenching of irradiation losses of plasmon polaritons in the chain to the level of only ohmic attenuation. The plasmon polariton dispersion and the group velocity of plasmon polariton wave packets were examined with respect to nano-sphere and chain parameters and mode polarization. Previous numerical results related to long-range plasmon polariton propagation in the chain are transparently interpreted within the analytical approach.

Dynamics of coupled plasmon polariton wave packets excited at a subwavelength slit in optically thin metal films

We study by numerical simulations the excitation and propagation dynamics of coupled surface plasmon polariton (SPP) wave packets (WPs) in optically thin Ag films and a bulk Ag/vacuum interface under the illumination of a subwavelength slit by 400 nm continuous wave (cw) and femtosecond pulsed light. The generated surface fields include contributions from both SPPs and quasicylindrical waves, which dominate in different regimes. We explore aspects of the coupled SPP modes in Ag thin films, including symmetry, propagation, attenuation, and the variation of coupling with incident angle and film thickness. Simulations of the electromagnetic transients initiated with femtosecond pulses reveal new features of coupled SPP WP generation and propagation in thin Ag films. Our results show that, under pulsed excitation, the SPP modes in an Ag thin film break up into two distinct bound surface wave packets characterized by marked differences in symmetries, group velocities, attenuation lengths, and dispersion properties. The nanometer spatial and femtosecond temporal scale excitation and propagation dynamics of the coupled SPP WPs are revealed in detail by movies recording the evolution of their transient field distributions.

Adiabatic Nanofocusing on Ultrasmooth Single-Crystalline Gold Tapers Creates a 10-nm-Sized Light Source with Few-Cycle Time Resolution

We demonstrate adiabatic nanofocusing of few-cycle light pulses using ultrasharp and ultrasmooth single-crystalline gold tapers. We show that the grating-induced launching of spectrally broad-band surface plasmon polariton wavepackets onto the shaft of such a taper generates isolated, point-like light spots with 10 fs duration and 10 nm diameter spatial extent at its very apex. This nanofocusing is so efficient that nanolocalized electric fields inducing strong optical nonlinearities at the tip end are reached with conventional high repetition rate laser oscillators. We use here the resulting second harmonic to fully characterize the time structure of the localized electric field in frequency-resolved interferometric autocorrelation measurements. Our results strongly suggest that these nanometer-sized ultrafast light spots will enable new experiments probing the dynamics of optical excitations of individual metallic, semiconducting, and magnetic nanostructures.

Adiabatic Nanofocusing Scattering-Type Optical Nanoscopy of Individual Gold Nanoparticles

We explore imaging of local electromagnetic fields in the vicinity of metallic nanoparticles using a grating-coupled scattering-type near-field scanning optical microscope. In this microscope, propagating surface plasmon polariton wavepackets are launched onto smooth gold tapers where they are adiabatically focused toward the nanometer-sized taper apex. We report two-dimensional raster-scanned optical images showing pronounced near-field contrast and demonstrating sub-30 nm resolution imaging of localized surface plasmon polariton fields of spherical and elliptical nanoparticles. By comparison to three-dimensional finite-difference time domain simulations, we conclude that virtually background-free near-field imaging is achieved. The microscope combines deep subwavelength resolution, high local field intensities and a straightforward imaging contrast, making it interesting for a variety of applications in linear and nonlinear nanospectroscopy.

Observation of few-cycle, strong-field phenomena in surface plasmon fields

We present experimental evidence of the generation of few-cycle propagating surface plasmon polariton wavepackets. These ultrashort plasmonic pulses comprised of only 2-3 field oscillations were characterized by an autocorrelation measurement based on electron photoemission. By exploiting plasmonic field enhancement, we achieved plasmon-induced tunnelling emission from the metal surface at low laser intensity, opening perspectives for strong-field experiments with low pulse energies. All-optical electron acceleration up to keV kinetic energy is also demonstrated in these surface-confined, few-cycle fields with only 1.35×10(12) W/cm2 focused laser intensity. The experimental results are found to be in excellent agreement with the model.