Periodic dielectric structures are typically integrated with a planar waveguide to create photonic band-edge modes for feedback in one-dimensional distributed feedback lasers and two-dimensional photonic-crystal lasers. Although photonic band-edge lasers are widely used in optics and biological applications, drawbacks include low modulation speeds and diffraction-limited mode confinement. In contrast, plasmonic nanolasers can support ultrafast dynamics and ultrasmall mode volumes. However, because of the large momentum mismatch between their nanolocalized lasing fields and free-space light, they suffer from large radiative losses and lack beam directionality. Here, we report lasing action from band-edge lattice plasmons in arrays of plasmonic nanocavities in a homogeneous dielectric environment. We find that optically pumped, two-dimensional arrays of plasmonic Au or Ag nanoparticles surrounded by an organic gain medium show directional beam emission (divergence angle <1.5° and linewidth <1.3 nm) characteristic of lasing action in the far-field, and behave as arrays of nanoscale light sources in the near-field. Using a semi-quantum electromagnetic approach to simulate the active optical responses, we show that lasing is achieved through stimulated energy transfer from the gain to the band-edge lattice plasmons in the deep subwavelength vicinity of the individual nanoparticles. Using femtosecond-transient absorption spectroscopy, we verified that lattice plasmons in plasmonic nanoparticle arrays could reach a 200-fold enhancement of the spontaneous emission rate of the dye because of their large local density of optical states.
Plasmonic lasers exploit strong electromagnetic field confinement at dimensions well below the diffraction limit. However, lasing from an electromagnetic hot spot supported by discrete, coupled metal nanoparticles (NPs) has not been explicitly demonstrated to date. We present a new design for a room-temperature nanolaser based on three-dimensional (3D) Au bowtie NPs supported by an organic gain material. The extreme field compression, and thus ultrasmall mode volume, within the bowtie gaps produced laser oscillations at the localized plasmon resonance gap mode of the 3D bowties. Transient absorption measurements confirmed ultrafast resonant energy transfer between photoexcited dye molecules and gap plasmons on the picosecond time scale. These plasmonic nanolasers are anticipated to be readily integrated into Si-based photonic devices, all-optical circuits, and nanoscale biosensors.
The optical and morphological characteristics of vanadium dioxide nanoparticles and thin films during their nucleation and growth phases have been studied by correlating the temperature and sharpness of the transition with the processing parameters. Thermal annealing results in grain growth and improved crystallinity. Normally, larger crystallites show smaller hysteresis, as there is a greater probability of finding a nucleating defect in the larger volume. But at the same time, this improved crystal perfection, which accompanies the thermal annealing and grain growth, tends to a larger hysteresis, as there are fewer nucleating defects within the volume. We show that the width and shape of the hysteresis cycle are thus determined by the competing effects of crystallinity and grain size.
We investigate the dielectric properties of a thin VO 2 film in the terahertz frequency range in the vicinity of the semiconductor-metal phase transition. Phase-sensitive broadband spectroscopy in the frequency region below the phonon bands of VO 2 gives insight into the conductive properties of the film during the phase transition. We compare our experimental data with models proposed for the evolution of the phase transition. The experimental data show that the phase transition occurs via the gradual growth of metallic domains in the film, and that the dielectric properties of the film in the vicinity of the transition temperature must be described by effective-medium theory. The simultaneous measurement of both transmission and phase shift allows us to show that Maxwell-Garnett effective-medium theory, coupled with the Drude conductivity model, can account for the observed behavior, whereas the widely used Bruggeman effective-medium theory is not consistent with our findings. Our results show that even at temperatures significantly above the transition temperature the formation of a uniform metallic phase is not complete.
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