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Surface plasmon polaritons (SPPs) are travelling surface waves that have shown promise for applications in nanophotonics as they provide a direct route toward photon-mediated electrical signal generation – a central paradigm for speeding up and scaling down photonic elements. SPP waves have also generated fundamental interest due to their high-field strength and sub-wavelength confinement, properties that have enabled the surface-enhanced Raman effect. Over the last decade, photoemission electron microscopy (PEEM) has emerged as a pioneering technique for imaging surface electric fields through ultrashort laser pulse mediated electron emission and has therefore become an indispensable tool for characterizing plasmonic phenomena at interfaces in a variety of materials. PEEM offers nanometer spatial resolution and femtosecond temporal resolution, allowing SPPs to be prepared, monitored, and manipulated on the nanometer-femtosecond scale. Through a brief review of recent reports, we aim to introduce PEEM-based SPP imaging and manipulation modalities and highlight their utility in the context of emerging nanoscale and quantum materials science advancements.

We demonstrate control over the spatial and temporal properties of surface plasmon polaritons (SPPs) launched from nanohole arrays in silver. The arrays provide wave vector matching to allow the conversion of free-space photons into counter-propagating SPPs. SPPs launched from multiple arrays interfere at well-defined spatial positions, and the interference fringes form an all-SPP periodic nano-optical grating which evolves in space and time as the SPPs propagate. The spatio-temporal characteristics of the optical grating can be tuned through various nanohole array parameters such as tilt angle, separation, and array width. In addition, we examine multiperiodic arrays (MPAs) consisting of arrays with different pitches placed adjacent to one another. This platform allows the temporal interference of SPPs with different central wavelengths to be tailored through the MPA geometric and structural parameters. The temporal interference serves as an encoded signal, whereby the frequency components can be controlled by the array properties.

Directional control over surface plasmon polariton (SPP) waves is a prerequisite for the development of miniaturized optical circuitry. Here, the efficacy of single and dual component SPP steering elements is explored through photoemission electron microscopy. Our imaging scheme relies on two-color photoemission and counter-propagating SPP generation, which collectively allow SPPs to be visualized in real space. Wave-vector difference mixing between the two-dimensional nanohole array and photon momenta enables SPP steering with directionality governed by the array lattice constant and input photon direction. In our dual component configuration, separate SPP generation and Bragg diffraction based steering optics are employed. We find that array Bragg planes principally influence the SPP angles through the array band structure, which allows us to visualize both positive and negative refractory waves. [ABSTRACT FROM AUTHOR]

Femtosecond transient reflectivity and absorption are used to measure the carrier lifetimes in alpha-Fe2O3 thin films and single crystals. In the hematite single crystal, the transient reflectivity displays oscillations due to the formation of longitudinal acoustic phonons generated following absorption of the ultrashot excitation pulse.

Observations on the luminescence of In2S3 and europium-doped In2S3 nanoparticles are presented. The resulting full-color emissions from these nanoparticles are also examined.

Strong upconversion luminescence of both Mn(super 2+) and Eu(super 3+) was observed in ZnS:Mn(super 2+), Eu(super 3+) codoped nanoparticles. Spectroscopic data and luminescence lifetime data indicated no evidence of energy transfer between Mn(super 2+) and Eu(super 3+) ions.

The formation and luminescence of a composite luminescent thin film composed of a aPPE blue polymer particles and ZnS/Mn (super 2+) doped nanoparticles with emission in the orange and its luminescence properties are described. Results show that due to temperature studies, ZnS/Mn (super 2+) particles in the nanocomposite significantly reduce the thermal quenching energy relative to that of bare ZnS/Mn (super 2+) nanoparticles.

A pulsed laser heating system has been developed that enables investigations of the dynamics and kinetics of nanoscale liquid films and liquid/solid interfaces on the nanosecond time scale in ultrahigh vacuum (UHV). Details of the design, implementation, and characterization of a nanosecond pulsed laser system for transiently heating nanoscale films are described. Nanosecond pulses from a Nd:YAG laser are used to rapidly heat thin films of adsorbed water or other volatile materials on a clean, well-characterized Pt(111) crystal in UHV. Heating rates of ~1010 K/s for temperature increases of ~100-200 K are obtained. Subsequent rapid cooling (~5 × 109 K/s) quenches the film, permitting insitu, post-heating analysis using a variety of surface science techniques. Lateral variations in the laser pulse energy are ~±2.7% leading to a temperature uncertainty of ~±4.4 K for a temperature jump of 200 K. Initial experiments with the apparatus demonstrate that crystalline ice films initially held at 90 K can be rapidly transformed into liquid water films with T > 273 K. No discernable recrystallization occurs during the rapid cooling back to cryogenic temperatures. In contrast, amorphous solid water films heated below the melting point rapidly crystallize. The nanosecond pulsed laser heating system can prepare nanoscale liquid and supercooled liquid films that persist for nanoseconds per heat pulse in an UHV environment, enabling experimental studies of a wide range of phenomena in liquids and at liquid/solid interfaces. [ABSTRACT FROM AUTHOR]

We describe a method for the generation of readily synchronizable, near-transform-limited, 1064-nm, 6-mJ pulses with Key words: Chirped pulse amplification, Nd:YAG regenerative amplifier.

We investigate the plasmonic properties of a self-assembled 2D array of Ag nanospheres (average particle diameter/inter-particle separation distance of 9/3.7 nm). The structures of the individual particles and their assemblies are characterized using high-resolution transmission electron microscopy (HR-TEM). The plasmonic response of the nanoparticle network is probed using two-photon photoemission electron microscopy (TP-PEEM). HR-TEM and TP-PEEM statistics reveal the structure and plasmonic response of the network to be homogeneous on average. This translates into a relatively uniform surface-enhanced Raman scattering (SERS) response from biphenyl,4-4'-dithiol (BPDT) molecules adsorbed onto different sites of the network. Reproducible, bright, and low-background SERS spectra are recorded and assigned on the basis of density functional theory calculations in which BPDT is chemisorbed onto the vertex of a finite tetrahedral Ag cluster consisting of 20 Ag atoms. A notable agreement between experiment and theory allows us to rigorously account for the observable vibrational states of BPDT in the ~200-2200 cm-1 region of the spectrum. Finite difference time domain simulations further reveal that physical enhancement factors on the order of 106 are attainable at the nanogaps formed between the silver nanospheres in the 2D array. Combined with modest chemical enhancement factors, this study paves the way for reproducible single molecule signals from an easily self-assembled SERS substrate. [ABSTRACT FROM AUTHOR]

We demonstrate control over the spatial and temporal properties of surface plasmon polaritons (SPPs) launched from nanohole arrays in silver. The arrays provide wave vector matching to allow the conversion of free-space photons into counter-propagating SPPs. SPPs launched from multiple arrays interfere at well-defined spatial positions, and the interference fringes form an all-SPP periodic nano-optical grating which evolves in space and time as the SPPs propagate. The spatio-temporal characteristics of the optical grating can be tuned through various nanohole array parameters such as tilt angle, separation, and array width. In addition, we examine multiperiodic arrays (MPAs) consisting of arrays with different pitches placed adjacent to one another. This platform allows the temporal interference of SPPs with different central wavelengths to be tailored through the MPA geometric and structural parameters. The temporal interference serves as an encoded signal, whereby the frequency components can be controlled by the array properties. [ABSTRACT FROM AUTHOR]

We use multi-photon photoemission electron microscopy (PEEM) to image the enhanced electric fields of silver nanoparticles supported on a silver thin film substrate. Electromagnetic field enhancement is measured by comparing the photoelectron yield of the nanoparticles with respect to the photoelectron yield of the surrounding silver thin film. We investigate the dependence of the photoelectron yield of the nanoparticle as a function of size and shape. Multi-photon PEEM results are presented for three average nanoparticle diameters: 34, 75, and 122 nm. The enhancement in photoelectron yield of single nanoparticles illuminated with femtosecond laser pulses (400 nm, ∼3.1 eV) is found to be a factor of 102 to 103 times greater than that produced by the flat silver thin film. High-resolution, multi-photon PEEM images of single silver nanoparticles reveal that the greatest enhancement in photoelectron yield is localized at distinct regions near the surface of the nanoparticle whose magnitude and spatial extent is dependent on the incident electric field polarization. In conjunction with correlated scanning electron microscopy (SEM), nanoparticles that deviate from nominally spherical shapes are found to exhibit irregular spatial distributions in the multi-photon PEEM images that are correlated with the unique shape and topology of the nanoparticle. [ABSTRACT FROM AUTHOR]

The ability to achieve sub-wavenumber resolution (0.6 cm-1) and a large signal-to-noise ratio in high-resolution broadband sum-frequency generation vibrational spectroscopy (HR-BB-SFG-VS) allows for the detailed SFG spectral lineshapes to be used in the unambiguous determination of fine spectral features. Changes in the structural spectroscopic phase in SFG-VS as a function of beam polarization and experimental geometry proved to be instrumental in the identification of an unexpected 2.78 ± 0.07 cm-1 spectral splitting for the two methyl groups at the vapor/dimethyl sulfoxide (DMSO, (CH3)2SO) liquid interface as well as in the determination of their orientational angles. [ABSTRACT FROM AUTHOR]