Experimental and Ab Initio Ultrafast Carrier Dynamics in Plasmonic Nanoparticles.

Ultrafast pump-probe measurements of plasmonic nanostructures probe the nonequilibrium behavior of excited carriers, which involves several competing effects obscured in typical empirical analyses. Here we present pump-probe measurements of plasmonic nanoparticles along with a complete theoretical description based on first-principles calculations of carrier dynamics and optical response, free of any fitting parameters. We account for detailed electronic-structure effects in the density of states, excited carrier distributions, electron-phonon coupling, and dielectric functions that allow us to avoid effective electron temperature approximations. Using this calculation method, we obtain excellent quantitative agreement with spectral and temporal features in transient-absorption measurements. In both our experiments and calculations, we identify the two major contributions of the initial response with distinct signatures: short-lived highly nonthermal excited carriers and longer-lived thermalizing carriers.

Clonal Clustering Using 10-Gene Multilocus Sequence Typing Reveals an Association Between Genotype and Listeria monocytogenes Maximum Growth Rate in Defined Medium.

We used a 10-gene (10G) multilocus sequence typing scheme to investigate the diversity and phylogenetic distribution of 124 Listeria monocytogenes strains across major lineages, major serotypes, and seven epidemic clones that have been previously associated with outbreaks. The 124 isolates proved to be diverse, with a total of 81 sequence types (10G-STs) belonging to 13 clonal complexes (CCs), where all STs of the same CC differ from one another in up to 3 of the 10 alleles (named as 10G-triple-locus-variant-clonal-complexes [10G-TLV-CCs]). Phenotypic characterization for 105 of the 124 strains showed that L. monocytogenes had variable maximum growth rate (µ(max)) in a defined medium at 16°C, and classification by lineage or serotype was not able to reflect the genetic basis for the difference of this phenotype. Among the six major 10G-TLV-CCs, 10G-TLV-CC4 that included lineage I strains had significantly lower µ(max) (Tukey honestly significant difference adjusted [adj.] p < 0.05) compared to 10G-TLV-CC1 and 10G-TLV-CC3 that both comprised lineage II strains, indicating a distinct difference in growth of these L. monocytogenes isolates under nutrient-limited conditions among some of the CCs. However, the other three (10G-TLV-CC2, 6, and 10) of the six major 10G-TLV-CCs containing either lineage I or lineage II strains did not show significantly different µ(max) compared to the others (adj. p < 0.05). Our findings highlighted the importance of using molecular typing methods that can be used in evolutionary analyses as a framework for further understanding the phenotypic characteristics of subgroups of L. monocytogenes.

Tuning the color of silicon nanostructures.

Empowering silicon (Si) with optical functions constitutes a very important challenge in photonics. The scalable fabrication capabilities for this earth-abundant, environmentally friendly material are unmatched in sophistication and can be unleashed to realize a plethora of high-performance photonic functionalities that find application in information, bio-, display, camouflage, ornamental, and energy technologies. Nanofashioning represents a general strategy to turn Si into a useful optical material and Si structures have already been engineered to enable light emission, optical cloaking, waveguiding, nonlinear optics, enhanced light absorption, and sensing. Here, we demonstrate that a wide spectrum of colors can be generated by harnessing the strong resonant light scattering properties of Si nanostructures under white light illumination. The ability to engineer such colors in a predetermined fashion through a choice of the structure size, dielectric environment, and illumination conditions opens up entirely new applications of Si and puts this material in a new light.

Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry.

The behavior of metals across a broad frequency range from microwave to ultraviolet frequencies is of interest in plasmonics, nanophotonics, and metamaterials. Depending on the frequency, losses of collective excitations in metals can be predominantly classical resistive effects or Landau damping. In this context, we present first-principles calculations that capture all of the significant microscopic mechanisms underlying surface plasmon decay and predict the initial excited carrier distributions so generated. Specifically, we include ab initio predictions of phonon-assisted optical excitations in metals, which are critical to bridging the frequency range between resistive losses at low frequencies and direct interband transitions at high frequencies. In the commonly used plasmonic materials, gold, silver, copper, and aluminum, we find that resistive losses compete with phonon-assisted carrier generation below the interband threshold, but hot carrier generation via direct transitions dominates above threshold. Finally, we predict energy-dependent lifetimes and mean free paths of hot carriers, accounting for electron-electron and electron-phonon scattering, to provide insight toward transport of plasmonically generated carriers at the nanoscale.

Nanophotonics. Plasmoelectric potentials in metal nanostructures.

The conversion of optical power to an electric potential is of general interest for energy applications and is typically obtained via optical excitation of semiconductor materials. We developed a method for achieving electric potential that uses an all-metal geometry based on the plasmon resonance in metal nanostructures. In arrays of gold nanoparticles on an indium tin oxide substrate and arrays of 100-nanometer-diameter holes in 20-nanometer-thick gold films on a glass substrate, we detected negative and positive surface potentials during monochromatic irradiation at wavelengths below or above the plasmon resonance, respectively. We observed plasmoelectric surface potentials as large as 100 millivolts under illumination of 100 milliwatts per square centimeter. Plasmoelectric devices may enable the development of all-metal optoelectronic devices that can convert light into electrical energy.