Direct Measurement of the Local Density of Optical States in the Time Domain.

One of the most fundamental and relevant properties of a photonic system is the local density of optical states (LDOS) as it defines the rate at which an excited emitter dissipates energy by coupling to its surrounding. However, the direct determination of the LDOS is challenging as it requires measurements of the complex electric field of a point dipole at its own position. We introduce here a near-field setup which can measure the terahertz electric field amplitude at the position of a point source in the time domain. From the measured amplitude, the frequency-dependent imaginary component of the electric field can be determined and the LDOS can be retrieved. As a proof of concept, this setup has been used to measure the partial LDOS (the LDOS for a defined dipole orientation) as a function of the distance to planar interfaces made of gold, InSb, and quartz. Furthermore, the spatially dependent partial LDOS of a resonant gold rod has been measured as well. These results have been compared with analytical results and simulations. The excellent agreement between measurements and theory demonstrates the applicability of this setup for the quantitative determination of the LDOS in complex photonic systems.

Room Temperature Exciton-Polariton Condensation in Silicon Metasurfaces Emerging from Bound States in the Continuum.

We show the first experimental demonstration of room-temperature exciton-polariton (EP) condensation from a bound state in the continuum (BIC). This demonstration is achieved by strongly coupling stable excitons in an organic perylene dye with the extremely long-lived BIC in a dielectric metasurface of silicon nanoparticles. The long lifetime of the BIC, mainly due to the suppression of radiation leakage, allows for EP thermalization to the ground state before decaying. This property results in a condensation threshold of less than 5 µJ cm-2, 1 order of magnitude lower than the lasing threshold reported in similar systems in the weak coupling limit.

Highly Ordered Supramolecular Materials of Phase-Separated Block Molecules for Long-Range Exciton Transport.

Efficient energy transport over long distances is essential for optoelectronic and light-harvesting devices. Although self-assembled nanofibers of organic molecules are shown to exhibit long exciton diffusion lengths, alignment of these nanofibers into films with large, organized domains with similar properties remains a challenge. Here, it is shown how the functionalization of C3 -symmetric carbonyl-bridged triarylamine trisamide (CBT) with oligodimethylsiloxane (oDMS) side chains of discrete length leads to fully covered surfaces with aligned domains up to 125 × 70 µm2 in which long-range exciton transport takes place. The nanoscale morphology within the domains consists of highly ordered nanofibers with discrete intercolumnar spacings within a soft amorphous oDMS matrix. The oDMS prevents bundling of the CBT fibers, reducing the number of defects within the CBT columns. As a result, the columns have a high degree of coherence, leading to exciton diffusion lengths of a few hundred nanometers with exciton diffusivities (≈0.05 cm2 s-1 ) that are comparable to those of a crystalline tetracene. These findings represent the next step toward fully covered surfaces of highly aligned nanofibers through functionalization with oDMS.

High-Frequency Sheet Conductance of Nanolayered WS2 Crystals for Two-Dimensional Nanodevices.

Time-resolved terahertz (THz) spectroscopy is a powerful technique for the determination of charge transport properties in photoexcited semiconductors. However, the relatively long wavelengths of THz radiation and the diffraction limit imposed by optical imaging systems reduce the applicability of THz spectroscopy to large samples with dimensions in the millimeter to centimeter range. Exploiting THz near-field spectroscopy, we present the first time-resolved THz measurements on a single exfoliated 2D nanolayered crystal of a transition metal dichalcogenide (WS2). The high spatial resolution of THz near-field spectroscopy enables mapping of the sheet conductance for an increasing number of atomic layers. The single-crystalline structure of the nanolayered crystal allows for the direct observation of low-energy phonon modes, which are present in all thicknesses, coupling with free carriers. Density functional theory calculations show that the phonon mode corresponds to the breathing mode between atomic layers in the weakly bonded van der Waals layers, which can be strongly influenced by substrate-induced strain. The non-invasive and high-resolution mapping technique of carrier dynamics in nanolayered crystals by time-resolved THz time domain spectroscopy enables possibilities for the investigation of the relation between phonons and charge transport in nanoscale semiconductors for applications in two-dimensional nanodevices.

Impact of indirect transitions on valley polarization in WS2 and WSe2.

Controlling the momentum of carriers in semiconductors, known as valley polarization, is a new resource for optoelectronics and information technologies. Materials exhibiting high polarization are needed for valley-based devices. Few-layer WS2 shows a remarkable spin-valley polarization above 90%, even at room temperature. In stark contrast, polarization is absent for few-layer WSe2 despite the expected material similarities. Here, we explain the origin of valley polarization in both materials based on the interplay between two indirect optical transitions. We show that the relative energy minima at the Λ- and K-valleys in the conduction band determine the spin-valley polarization of the direct K-K transition. Polarization appears as the energy of the K-valley rises above the Λ-valley as a function of temperature and number of layers. Our results advance the understanding of the high spin-valley polarization in WS2. This insight will impact the design of both passive and tunable valleytronic devices operating at room temperature.

Chasing Vibro-Polariton Fingerprints in Infrared and Raman Spectra Using Surface Lattice Resonances on Extended Metasurfaces.

We present an experimental investigation of vibrational strong coupling of C=O bonds in poly(methyl methacrylate) to surface lattice resonances (SLRs) on arrays of gold particles in infrared and Raman spectra. SLRs are generated from the enhanced radiative coupling of localized resonances in single particles by diffraction in the array. Compared to previous studies in Fabry-Perot cavities, particle arrays provide a fully open system that easily couples with external radiation while having large field confinement close to the array. We control the coupling by tuning the period of the array, as evidenced by the splitting of the C=O vibration resonance in the lower and upper vibro-polaritons of the IR extinction spectra. Despite clear evidence of vibrational strong coupling in IR transmission spectra, both Raman spectroscopy and micro-Raman mapping do not show any polariton signatures. Our results suggest that the search for vibrational strong coupling in Raman spectra may need alternative cavity designs or a different experimental approach.

Unveiling the Symmetry Protection of Bound States in the Continuum with Terahertz Near-Field Imaging.

Bound states in the continuum (BICs) represent a new paradigm in photonics due to the full suppression of radiation losses. However, this suppression has also hampered the direct observation of them. By using a double terahertz (THz) near-field technique that allows the local excitation and detection of the THz amplitude, we are able to map for the first time the electromagnetic field amplitude and phase of BICs over extended areas, unveiling the field-symmetry protection that suppresses the far-field radiation. This investigation, done for metasurfaces of dimer scatterers, reveals the in-plane extension and formation of BICs with antisymmetric phases, in agreement with coupled-dipole calculations. By displacing the scatterers, we show experimentally that a mirror symmetry is not a necessary condition for a BIC formation. Only π-rotation symmetry is required, making BICs exceptionally robust to structural changes. This work makes the local field of BICs experimentally accessible, which is crucial for the engineering of cavities with infinite lifetimes.

Spatial coherence from Nd3+ quantum emitters mediated by a plasmonic chain.

Controlling the coherence properties of rare earth emitters in solid-state platforms in the absence of an optical cavity is highly desirable for quantum light-matter interfaces and photonic networks. Here, we demonstrate the possibility of generating directional and spatially coherent light from Nd3+ ions coupled to the longitudinal plasmonic mode of a chain of interacting Ag nanoparticles. The effect of the plasmonic chain on the Nd3+ emission is analyzed by Fourier microscopy. The results reveal the presence of an interference pattern in which the Nd3+ emission is enhanced at specific directions, as a distinctive signature of spatial coherence. Numerical simulations corroborate the need of near-field coherent coupling of the emitting ions with the plasmonic chain mode. The work provides fundamental insights for controlling the coherence properties of quantum emitters at room temperature and opens new avenues towards rare earth based nanoscale hybrid devices for quantum information or optical communication in nanocircuits.

Fröhlich interaction dominated by a single phonon mode in CsPbBr3.

The excellent optoelectronic performance of lead halide perovskites has generated great interest in their fundamental properties. The polar nature of the perovskite lattice means that electron-lattice coupling is governed by the Fröhlich interaction. Still, considerable ambiguity exists regarding the phonon modes that participate in this crucial mechanism. Here, we use multiphonon Raman scattering and THz time-domain spectroscopy to investigate Fröhlich coupling in CsPbBr3. We identify a longitudinal optical phonon mode that dominates the interaction, and surmise that this mode effectively defines exciton-phonon scattering in CsPbBr3, and possibly similar materials. It is additionally revealed that the observed strength of the Fröhlich interaction is significantly higher than the expected intrinsic value for CsPbBr3, and is likely enhanced by carrier localization in the colloidal perovskite nanocrystals. Our experiments also unearthed a dipole-related dielectric relaxation mechanism which may impact transport properties.

Effective Negative Diffusion of Singlet Excitons in Organic Semiconductors.

Using diffraction-limited ultrafast imaging techniques, we investigate the propagation of singlet and triplet excitons in single-crystal tetracene. Instead of an expected broadening, the distribution of singlet excitons narrows on a nanosecond time scale after photoexcitation. This narrowing results in an effective negative diffusion in which singlet excitons migrate toward the high-density region, eventually leading to a singlet exciton distribution that is smaller than the laser excitation spot. Modeling the excited-state dynamics demonstrates that the origin of the anomalous diffusion is rooted in nonlinear triplet-triplet annihilation (TTA). We anticipate that this is a general phenomenon that can be used to study exciton diffusion and nonlinear TTA rates in semiconductors relevant for organic optoelectronics.

Correlated Exciton Fluctuations in a Two-Dimensional Semiconductor on a Metal.

Excitons in nanoscale materials can exhibit fluorescence fluctuations. Intermittency is pervasive in zero-dimensional emitters such as single molecules and quantum dots. In contrast, two-dimensional semiconductors are generally regarded as stable light sources. Noise contains, however, valuable information about a material. Here, we demonstrate fluorescence fluctuations in a monolayer semiconductor due to sensitivity to its nanoscopic environment focusing on the case of a metal film. The fluctuations are spatially correlated over tens of micrometers and follow power-law statistics, with simultaneous changes in emission intensity and lifetime. At low temperatures, an additional spectral contribution from interface trap states emerges with fluctuations that are correlated with neutral excitons and anticorrelated with trions. Mastering exciton fluctuations has implications for light-emitting devices such as single-photon sources and could lead to novel excitonic sensors. The quantification of fluorescence fluctuations, including imaging, unlocks a set of promising tools to characterize and exploit two-dimensional semiconductors and their interfaces.

Ultrafast Dynamics of Nonequilibrium Organic Exciton-Polariton Condensates.

Exciton-polariton condensation in organic materials, arising from the coupling of Frenkel excitons to the electromagnetic field in cavities, is a phenomenon resulting in low-threshold coherent light emission among other fascinating properties. The exact mechanisms leading to the thermalization of organic exciton-polaritons toward condensation are not yet understood, partly due to the complexity of organic molecules and partly to the canonical microcavities used in condensation studies, which limit broadband studies. Here, we exploit an entirely different cavity design, i.e., an array of plasmonic nanoparticles strongly coupled to organic molecules, to successfully measure the broadband ultrafast dynamics of the strongly coupled system. Sharp features emerge in the transient spectrum originating from the formation of a condensate with a well-defined molecular vibrational composition. These measurements represent the first direct experimental evidence that molecular vibrations drive condensation in organic systems and provide a benchmark for modeling the dynamics of organic-based exciton-polariton condensates.

Coherent Control of the Optical Absorption in a Plasmonic Lattice Coupled to a Luminescent Layer.

We experimentally demonstrate the coherent control, i.e., phase-dependent enhancement and suppression, of the optical absorption in an array of metallic nanoantennas covered by a thin luminescent layer. The coherent control is achieved by using two collinear, counterpropagating, and phase-controlled incident waves with wavelength matching the absorption spectrum of dye molecules coupled to the array. Symmetry arguments shed light on the relation between the relative phase of the incident waves and the excitation efficiency of the optical resonances of the system. This coherent control is associated with a phase-dependent distribution of the electromagnetic near fields in the structure which enables a significant reduction of the unwanted dissipation in the metallic structures.

Directional sideward emission from luminescent plasmonic nanostructures.

Periodic arrays of metallic nanoparticles can be used to enhance the emission of light in certain directions. We fabricated hexagonal arrays of aluminium nanoparticles combined with thin layers of luminescent material and optimized period (275 nm) and thickness (1500 nm) to obtain sideward directional emission into glass for a wavelength band around 620 nm. The key physics is that the luminescent layer acts as a waveguide, from which light is emitted at preferential angles using diffractive effects. This phenomenon has applications in the field of solid-state lighting, where there is a desire for small, bright and directional sources.

Enhanced THz extinction in arrays of resonant semiconductor particles.

We demonstrate experimentally the enhanced THz extinction by periodic arrays of resonant semiconductor particles. This phenomenon is explained in terms of the radiative coupling of localized resonances with diffractive orders in the plane of the array (Rayleigh anomalies). The experimental results are described by numerical calculations using a coupled dipole model and by Finite-Difference in Time-Domain simulations. An optimum particle size for enhancing the extinction efficiency of the array is found. This optimum is determined by the frequency detuning between the localized resonances in the individual particles and the Rayleigh anomaly. The extinction calculations and measurements are also compared to near-field simulations illustrating the optimum particle size for the enhancement of the near-field.

Modulated light absorption and emission of a luminescent layer by phase-controlled multiple beam illumination.

We propose a multiple beam illumination scheme to control the intensity of the light emitted by a thin luminescent layer. The experiment is designed to get as close as possible to the condition of Coherent Perfect Absorption (CPA) at a wavelength at which the absorption coefficient of the luminescent layer is low, and it is realized by externally acting on the phase difference between the incident beams. We elucidate experimental limitations that prevent the achievement of CPA in these slabs. Nevertheless, we are able to demonstrate that when the two beams destructively interfere outside the luminescent layer, the incident light is more efficiently absorbed by the luminescent layer and the intensity of the emitted light is phase-modulated.

Nanowire antenna absorption probed with time-reversed fourier microscopy.

Understanding light absorption in individual nanostructures is crucial for optimizing the light-matter interaction at the nanoscale. Here, we introduce a technique named time-reversed Fourier microscopy that enables the measurement of the angle-dependent light absorption in dilute arrays of uncoupled semiconductor nanowires. Because of their large separation, the nanowires have a response that can be described in terms of individual nanostructures. The geometry of individual nanowires makes them behave as nanoantennas that show a strong interaction with the incident light. The angle-dependent absorption measurements, which are compared to numerical simulations and Mie scattering calculations, show the transition from guided-mode to Mie-resonance absorption in individual nanowires and the relative efficiency of these two absorption mechanisms in the same nanostructures. Mie theory fails to describe the absorption in finite-length vertical nanowires illuminated at small angles with respect to their axis. At these angles, the incident light is efficiently absorbed after being coupled to guided modes. Our findings are relevant for the design of nanowire-based photodetectors and solar cells with an optimum efficiency.

Modified light emission from emitters coupled to long-range guided modes in strongly absorbing layers.

We demonstrate the near-field coupling and energy transfer between photoexcited dye molecules and guided modes in layers of strongly absorbing dielectrics. The dye molecules decay by exciting long-range guided modes (LRGMs) in a thin layer of chalcogenide glass. These modes can exist in spite of the very large absorption of the material forming the layer. The LRGMs are detected by coupling then out to free space radiation through a prism in the Krestschmann configuration. By calculating the dissipated power of a dipole, representing a dye molecule, in the vicinity of the absorbing thin film, we show that there is a large probability of decay exciting LRGMs. This probability can reach 35% for perpendicularly oriented dipoles. The demonstration of the excitation of LRGMs in thin films of absorbing dielectrics by near-field coupling of excited molecules opens the possibility to compensate for the losses in the propagation of these modes.

Long-range guided THz radiation by thin layers of water.

We propose a novel method to guide THz radiation with low losses along thin layers of water. This approach is based on the coupling of evanescent surface fields at the opposite sides of the thin water layer surrounded by a dielectric material, which leads to a maximum field amplitude at the interfaces and a reduction of the energy density inside the water film. In spite of the strong absorption of water in this frequency range, calculations show that the field distribution can lead to propagation lengths of several centimeters. By means of attenuated total reflection measurements we demonstrate the coupling of incident THz radiation to the long-range surface guided modes across a layer of water with a thickness of 24 µm. This first demonstration paves the way for THz sensing in aqueous environments.

Selective detection of bacterial layers with terahertz plasmonic antennas.

Current detection and identification of micro-organisms is based on either rather unspecific rapid microscopy or on more accurate but complex and time-consuming procedures. In a medical context, the determination of the bacteria Gram type is of significant interest. The diagnostic of microbial infection often requires the identification of the microbiological agent responsible for the infection, or at least the identification of its family (Gram type), in a matter of minutes. In this work, we propose to use terahertz frequency range antennas for the enhanced selective detection of bacteria types. Several microorganisms are investigated by terahertz time-domain spectroscopy: a fast, contactless and damage-free investigation method to gain information on the presence and the nature of the microorganisms. We demonstrate that plasmonic antennas enhance the detection sensitivity for bacterial layers and allow the selective recognition of the Gram type of the bacteria.