Ultrafast optical properties of stoichiometric and non-stoichiometric refractory metal nitrides TiNx, ZrNx, and HfNx.

Refractory metal nitrides have recently gained attention in various fields of modern photonics due to their cheap and robust production technology, silicon-technology compatibility, high thermal and mechanical resistance, and competitive optical characteristics in comparison to typical plasmonic materials like gold and silver. In this work, we demonstrate that by varying the stoichiometry of sputtered nitride films, both static and ultrafast optical responses of refractory metal nitrides can efficiently be controlled. We further prove that the spectral changes in ultrafast transient response are directly related to the position of the epsilon-near-zero region. At the same time, the analysis of the temporal dynamics allows us to identify three time components: the "fast" femtosecond one, the "moderate" picosecond one, and the "slow" at the nanosecond time scale. We also find out that the non-stoichiometry does not significantly decrease the recovery time of the reflectance value. Our results show the strong electron-phonon coupling and reveal the importance of both the electron and lattice temperature-induced changes in the permittivity near the ENZ region and the thermal origin of the long tail in the transient optical response of refractory nitrides.

Role of Self-Trapped Excitons in the Broadband Emission of Lead-Free Perovskite-Inspired Cu2AgBiI6.

The perovskite-inspired Cu2AgBiI6 (CABI) absorber shows promise for low-toxicity indoor photovoltaics. However, the carrier self-trapping in this material limits its photovoltaic performance. Herein, we examine the self-trapping mechanism in CABI by analyzing the excited-state dynamics of its absorption band at 425 nm, which is responsible for the self-trapped exciton emission, using a combination of photoluminescence and ultrafast transient absorption spectroscopies. Photoexcitation in CABI rapidly generates charge carriers in the silver iodide lattice sites, which localize into the self-trapped states and luminesce. Furthermore, a Cu-Ag-I-rich phase that exhibits similar spectral responses as CABI is synthesized, and a comprehensive structural and photophysical study of this phase provides insights into the nature of the excited states of CABI. Overall, this work explains the origin of self-trapping in CABI. This understanding will play a crucial role in optimizing its optoelectronic properties. It also encourages compositional engineering as the key to suppressing self-trapping in CABI.

Unveiling Long-Lived Hot-Electron Dynamics via Hyperbolic Meta-antennas.

Conventional plasmonic nanoantennas enable scattering and absorption bands at the same wavelength region, making their utilization to full potential impossible for both features simultaneously. Here, we take advantage of spectrally separated scattering and absorption resonance bands in hyperbolic meta-antennas (HMA) to enhance the hot-electron generation and prolong the relaxation dynamics of hot carriers. First, we show that HMA enables extending plasmon-modulated photoluminescence spectrum toward longer wavelengths due to its particular scattering spectrum, in comparison to the corresponding nanodisk antennas (NDA). Then, we demonstrate that the tunable absorption band of HMA controls and modifies the lifetime of the plasmon-induced hot electrons with enhanced excitation efficiency in the near-infrared region and also broadens the utilization of the visible/NIR spectrum in comparison to NDA. Thus, the rational heterostructures designed by plasmonic and adsorbate/dielectric layers with such dynamics can be a platform for optimization and engineering the utilization of plasmon-induced hot carriers.

All-optical switching based on plasmon-induced Enhancement of Index of Refraction.

In quantum optical Enhancement of Index of Refraction (EIR), coherence and quantum interference render the atomic systems to exhibit orders of magnitude higher susceptibilities with vanishing or even negative absorption at their resonances. Here we show the plasmonic analogue of the quantum optical EIR effect in an optical system and further implement this in a linear all-optical switching mechanism. We realize plasmon-induced EIR using a particular plasmonic metasurface consisting of a square array of L-shaped meta-molecules. In contrast to the conventional methods, this approach provides a scheme to modulate the amplitude of incident signals by coherent control of absorption without implementing gain materials or nonlinear processes. Therefore, light is controlled by applying ultra-low intensity at the extreme levels of spatiotemporal localization. In the pursuit of potential applications of linear all-optical switching devices, this scheme may introduce an effective tool for improving the modulation strength of optical modulators and switches through the amplification of input signals at ultra-low power.

Full three-dimensional Poynting vector flow analysis of great field-intensity enhancement in specifically sized spherical-particles.

The Poynting vector plays a key role in electrodynamics as it is directly related to the power and the momentum carried by an electromagnetic wave. Based on the Lorenz-Mie theory, we report on the focusing effect of a spherical particle-lens by properly analysing the Poynting vector maps. Conventional two-dimensional (2D) maps showing Poynting vector magnitude and direction in a given plane cannot deliver information on three-dimensional (3D) directivity and vectorisation in key regions of singularities, such as vortexes and saddle points, due to poor expressiveness. In this article, an analytical 3D mapping technology is utilised to track the field-features passing through the singularities of the distribution of the Poynting vector in a spherically dielectric mesoscale particle-lens. We discovered that the spheres with the certain size parameters can stimulate extremely large field-intensity at singularities and then form two circular hotspots around the sphere poles. An astonishing large 'heart-shape' 3D Poynting vector circulation, which cannot be predicted by conventional 2D mapping analysis, is found to provide a great angular variation within an enormous range in these spheres. We anticipate that this effect will contribute to the field-enhancement phenomena, such as surface enhances Raman scattering, surface enhances absorption, super-resolution imaging and others.

High order Fano resonances and giant magnetic fields in dielectric microspheres.

We show that weakly dissipating dielectric spheres made of materials such as glass, quartz, etc. can support high order Fano resonances associated with internal Mie modes. These resonances, happening for specific values of the size parameter, yield field-intensity enhancement factors on the order of 104-107, which can be directly obtained from analytical calculations. Associated to these "super-resonances", we analyze the emergence of magnetic nanojets with giant magnetic fields, which might be attractive for many photonic applications.

Extraordinary Effects in Quasi-Periodic Gold Nanocavities: Enhanced Transmission and Polarization Control of Cavity Modes.

Plasmonic quasi-periodic structures are well-known to exhibit several surprising phenomena with respect to their periodic counterparts, due to their long-range order and higher rotational symmetry. Thanks to their specific geometrical arrangement, plasmonic quasi-crystals offer unique possibilities in tailoring the coupling and propagation of surface plasmons through their lattice, a scenario in which a plethora of fascinating phenomena can take place. In this paper we investigate the extraordinary transmission phenomenon occurring in specifically patterned Thue-Morse nanocavities, demonstrating noticeable enhanced transmission, directly revealed by near-field optical experiments, performed by means of a scanning near-field optical microscope (SNOM). SNOM further provides an intuitive picture of confined plasmon modes inside the nanocavities and confirms that localization of plasmon modes is based on size and depth of nanocavities, while cross talk between close cavities via propagating plasmons holds the polarization response of patterned quasi-crystals. Our performed numerical simulations are in good agreement with the experimental results. Thus, the control on cavity size and incident polarization can be used to alter the intensity and spatial properties of confined cavity modes in such structures, which can be exploited in order to design a plasmonic device with customized optical properties and desired functionalities, to be used for several applications in quantum plasmonics.