Two-photon absorption in silicon using the real density matrix approach.

Two-photon absorption in indirect gap semiconductors is a frequently encountered, but not well-understood phenomenon. To address this, the real-density matrix approach is applied to describe two-photon absorption in silicon through the excitonic response to the interacting fields. This approach produces an analytical expression for the dispersion of the two-photon absorption coefficient for indirect-gap materials and can be used to explain trends in reported experimental data for bulk silicon both old and new with minimal fitting.

Extreme Electron-Photon Interaction in Disordered Perovskites.

The interaction of light with solids can be dramatically enhanced owing to electron-photon momentum matching. This mechanism manifests when light scattering from nanometer-sized clusters including a specific case of self-assembled nanostructures that form a long-range translational order but local disorder (crystal-liquid duality). In this paper, a new strategy based on both cases for the light-matter-interaction enhancement in a direct bandgap semiconductor - lead halide perovskite CsPbBr - by using electric pulse-driven structural disorder, is addressed.

Photon Momentum Enabled Light Absorption in Silicon.

Photons do not carry sufficient momentum to induce indirect optical transitions in semiconducting materials, such as silicon, necessitating the assistance of lattice phonons to conserve momentum. Compared to direct bandgap semiconductors, this renders silicon a less attractive material for a wide variety of optoelectronic applications. In this work, we introduce an alternative strategy to fulfill the momentum-matching requirement in indirect optical transitions.

Photon-Momentum-Enabled Electronic Raman Scattering in Silicon Glass.

The nature of enhanced photoemission in disordered and amorphous solids is an intriguing question. A point in case is light emission in porous and nanostructured silicon, a phenomenon that is still not fully understood. In this work, we study structural photoemission in heterogeneous cross-linked silicon glass, a material that represents an intermediate state between the amorphous and crystalline phases, characterized by a narrow distribution of structure sizes.

Light-Controlled Multiphase Structuring of Perovskite Crystal Enabled by Thermoplasmonic Metasurface.

Halide perovskites belong to an important family of semiconducting materials with electronic properties that enable a myriad of applications, especially in photovoltaics and optoelectronics. Their optical properties, including photoluminescence quantum yield, are affected and notably enhanced at crystal imperfections where the symmetry is broken and the density of states increases. These lattice distortions can be introduced through structural phase transitions, allowing charge gradients to appear near the interfaces between phase structures.

Designing two-dimensional temperature profiles using tunable thermoplasmonics.

Heat flow generation and manipulation in nanometer-sized solids using light represents one of the up-and-coming tasks in thermonanophotonics. Enhanced light-matter interaction due to plasmon resonance permits metallic nanostructures to absorb light energy efficiently, and it results in extra optical heating. The net temperature increment of nanostructures is directly dependent on heat exchange with a thermostat.

Nanoscale Melting of 3D Confined Azopolymers through Tunable Thermoplasmonics.

Phase transitions that are thermally induced by using light at the nanoscale play a vital role in material science. Enhanced optical heating sustained by resonant nanostructures can turn out to be insignificant when a higher thermal conductivity of a heatsink, regardless of the pumping intensity. In this Letter, we demonstrate an approach to control an operating temperature range due to excess heating of a structured heatsink.

Far-field Raman color superlensing based on disordered plasmonics.

Plasmon multiple scattering within a disordered metal-dielectric medium allows one to enhance a cubic susceptibility drastically, and thus stimulated Raman scattering (SRS) can occur in highly confined media exposed to the continuous-wave low-powered pump. In this study, a percolated 50 nm titanium oxynitride thin film is used as a disordered nonlinear metalens that meets epsilon-near-zero (ENZ) wavelengths in the visible and near infrared region. We experimentally demonstrate a far-field Raman superlensing effect by showing a subwavelength resolution of /6 at different SRS overtones using multiwalled carbon nanotubes directly dispersed on the metalens.

Disordered Nonlinear Metalens for Raman Spectral Nanoimaging.

Over the past decades, considerable progress has been made toward far-field optical imaging beyond the diffraction limit. However, most working proof-of-concepts are based on either time-consuming scanning of a subdiffraction focal spot over a sample or postrecovery treatment using information on a sought image. To our knowledge, none of these can be regarded as being close to a perfect far-field superlensing system capable of real-time color imaging with subwavelength resolution.

Superresolution stimulated Raman scattering microscopy using 2-ENZ nano-composites.

Superlensing plays a crucial role in near- and far-field optical imaging with sub-wavelength resolution. One of the ways to expand optical bandwidth is surface plasmon resonances in layered metal-dielectric nanostructures. These resonances are commonly excited at a tunable single frequency.

Near-field depolarization of tip-enhanced Raman scattering by single azo-chromophores.

The intrinsic symmetry and orientation of single molecules play a crucial role in enhanced optical spectroscopy and nanoscopic imaging. Unlike bulk materials, in which all molecular orientations are unavoidably averaged in the far-field, intensities of vibrational modes in tip-enhanced Raman scattering (TERS) depend greatly on the polarization direction of near-field light. It means that a near-field Raman "dichroism" becomes possible for anisotropic single molecules.

Nonlinear Raman Effects Enhanced by Surface Plasmon Excitation in Planar Refractory Nanoantennas.

We consider a nonlinear mechanism of localized light inelastic scattering within nanopatterned plasmonic and Raman-active titanium nitride (TiN) thin films exposed to continuous-wave (cw) modest-power laser light. Owing to the strong third-order nonlinear interaction between optically excited broadband surface plasmons and localized Stokes and anti-Stokes waves, both stimulated and inverse Raman effects can be observed. We provide experimental evidence for coherent amplification of the localized Raman signals using a planar square-shaped refractory antenna.

Near-field Raman dichroism of azo-polymers exposed to nanoscale dc electrical and optical poling.

Azobenzene-functionalized polymer films are functional materials, where the (planar vs. homeotropic) orientation of azo-dyes can be used for storing data. In order to characterize the nanoscale 3D orientation of the pigments in sub-10 nm thick polymer films we use two complementary techniques: polarization-controlled tip-enhanced Raman scattering (TERS) microscopy and contact scanning capacity microscopy.

Near-field optical taper antennas fabricated with a highly replicable ac electrochemical etching method.

This paper describes a novel chemical etching method to fabricate high quality near-field optical antennas-tapered metallic tips-from gold wire in a reproducible way for optically probing a specimen on the nanoscale. A new type of an electrochemical cell is introduced and different dc and ac etching regimes are studied in detail. The formation and dynamics of a meniscus around a gold wire immersed in an electrolyte when supplying a square wave voltage are considered.