Gradient-induced long-range optical pulling force based on photonic band gap.

Optical pulling provides a new degree of freedom in optical manipulation. It is generally believed that long-range optical pulling forces cannot be generated by the gradient of the incident field. Here, we theoretically propose and numerically demonstrate the realization of a long-range optical pulling force stemming from a self-induced gradient field in the manipulated object. In analogy to potential barriers in quantum tunnelling, we use a photonic band gap design in order to obtain the intensity gradients inside a manipulated object placed in a photonic crystal waveguide, thereby achieving a pulling force. Unlike the usual scattering-type optical pulling forces, the proposed gradient-field approach does not require precise elimination of the reflection from the manipulated objects. In particular, the Einstein-Laub formalism is applied to design this unconventional gradient force. The magnitude of the force can be enhanced by a factor of up to 50 at the optical resonance of the manipulated object in the waveguide, making it insensitive to absorption. The developed approach helps to break the limitation of scattering forces to obtain long-range optical pulling for manipulation and sorting of nanoparticles and other nano-objects. The developed principle of using the band gap to obtain a pulling force may also be applied to other types of waves, such as acoustic or water waves, which are important for numerous applications.

Large area single crystal gold of single nanometer thickness for nanophotonics.

Two-dimensional single crystal metals, in which the behavior of highly confined optical modes is intertwined with quantum phenomena, are highly sought after for next-generation technologies. Here, we report large area (>104 µm2), single crystal two-dimensional gold flakes (2DGFs) with thicknesses down to a single nanometer level, employing an atomic-level precision chemical etching approach. The decrease of the thickness down to such scales leads to the quantization of the electronic states, endowing 2DGFs with quantum-confinement-augmented optical nonlinearity, particularly leading to more than two orders of magnitude enhancement in harmonic generation compared with their thick polycrystalline counterparts. The nanometer-scale thickness and single crystal quality makes 2DGFs a promising platform for realizing plasmonic nanostructures with nanoscale optical confinement. This is demonstrated by patterning 2DGFs into nanoribbon arrays, exhibiting strongly confined near infrared plasmonic resonances with high quality factors. The developed 2DGFs provide an emerging platform for nanophotonic research and open up opportunities for applications in ultrathin plasmonic, optoelectronic and quantum devices.

Time-Dependent Ultrafast Quadratic Nonlinearity in an Epsilon-Near-Zero Platform.

Ultrafast nonlinearity, which results in modulation of the linear optical response, is a basis for the development of time-varying media, in particular those operating in the epsilon-near-zero (ENZ) regime. Here, we demonstrate that the intraband excitation of hot electrons in the ENZ film results in a second-harmonic resonance shift of ∼10 THz (40 nm) and second-harmonic generation (SHG) intensity changes of >100% with only minor (<1%) changes in linear transmission. The modulation is 10-fold enhanced by a plasmonic metasurface coupled to a film, allowing for ultrafast modulation of circularly polarized SHG. The effect is described by the plasma frequency renormalization in the ENZ material and the modification of the electron damping, with a possible influence of the hot-electron dynamics on the quadratic susceptibility. The results elucidate the nature of the second-order nonlinearity in ENZ materials and pave the way to the rational engineering of active nonlinear metamaterials and metasurfaces for time-varying applications.

Ultrafast hot-carrier dynamics in ultrathin monocrystalline gold.

Applications in photodetection, photochemistry, and active metamaterials and metasurfaces require fundamental understanding of ultrafast nonthermal and thermal electron processes in metallic nanosystems. Significant progress has been recently achieved in synthesis and investigation of low-loss monocrystalline gold, opening up opportunities for its use in ultrathin nanophotonic architectures. Here, we reveal fundamental differences in hot-electron thermalisation dynamics between monocrystalline and polycrystalline ultrathin (down to 10 nm thickness) gold films. Comparison of weak and strong excitation regimes showcases a counterintuitive unique interplay between thermalised and non-thermalised electron dynamics in mesoscopic gold with the important influence of the X-point interband transitions on the intraband electron relaxation. We also experimentally demonstrate the effect of hot-electron transfer into a substrate and the substrate thermal properties on electron-electron and electron-phonon scattering in ultrathin films. The hot-electron injection efficiency from monocrystalline gold into TiO2, approaching 9% is measured, close to the theoretical limit. These experimental and modelling results reveal the important role of crystallinity and interfaces on the microscopic electronic processes important in numerous applications.

Femtosecond laser modified metal surfaces alter biofilm architecture and reduce bacterial biofilm formation.

Biofilm formation, or microfouling, is a basic strategy of bacteria to colonise a surface and may happen on surfaces of any nature whenever bacteria are present. Biofilms are hard to eradicate due to the matrix in which the bacteria reside, consisting of strong, adhesive and adaptive self-produced polymers such as eDNA and functional amyloids. Targeting a biofilm matrix may be a promising strategy to prevent biofilm formation. Here, femtosecond laser irradiation was used to modify the stainless steel surface in order to introduce either conical spike or conical groove textures. The resulting topography consists of hierarchical nano-microstructures which substantially increase roughness. The biofilms of two model bacterial strains, P. aeruginosa PA01 and S. aureus ATCC29423, formed on such nanotextured metal surfaces, were considerably modified due to a substantial reduction in amyloid production and due to changes in eDNA surface adhesion, leading to significant reduction in biofilm biomass. Altering the topography of the metal surface, therefore, radically diminishes biofilm development solely by altering biofilm architecture. At the same time, growth and colonisation of the surface by eukaryotic adipose tissue-derived stem cells were apparently enhanced, leading to possible further advantages in controlling eukaryotic growth while suppressing prokaryotic contamination. The obtained results are important for developing anti-bacterial surfaces for numerous applications.

Multimode hybrid gold-silicon nanoantennas for tailored nanoscale optical confinement.

High-index dielectric nanoantennas, which provide an interplay between electric and magnetic modes, have been widely used as building blocks for a variety of devices and metasurfaces, both in linear and nonlinear regimes. Here, we investigate hybrid metal-semiconductor nanoantennas, consisting of a multimode silicon nanopillar core coated with a gold layer, that offer an enhanced degree of control over the mode selection and confinement, and emission of light on the nanoscale exploiting high-order electric and magnetic resonances. Cathodoluminescence spectra revealed a multitude of resonant modes supported by the nanoantennas due to hybridization of the Mie resonances of the core and the plasmonic resonances of the shell. Eigenmode analysis revealed the modes that exhibit enhanced field localization at the gold interface, together with high confinement within the nanopillar volume. Consequently, this architecture provides a flexible means of engineering nanoscale components with tailored optical modes and field confinement for a plethora of applications, including sensing, hot-electron photodetection and nanophotonics with cylindrical vector beams.

Waveguide-Integrated Light-Emitting Metal-Insulator-Graphene Tunnel Junctions.

Ultrafast interfacing of electrical and optical signals at the nanoscale is highly desired for on-chip applications including optical interconnects and data processing devices. Here, we report electrically driven nanoscale optical sources based on metal-insulator-graphene tunnel junctions (MIG-TJs), featuring waveguided output with broadband spectral characteristics. Electrically driven inelastic tunneling in a MIG-TJ, realized by integrating a silver nanowire with graphene, provides broadband excitation of plasmonic modes in the junction with propagation lengths of several micrometers (∼10 times larger than that for metal-insulator-metal junctions), which therefore propagate toward the junction edge with low loss and couple to the nanowire waveguide with an efficiency of ∼70% (∼1000 times higher than that for metal-insulator-metal junctions). Alternatively, lateral coupling of the MIG-TJ to a semiconductor nanowire provides a platform for efficient outcoupling of electrically driven plasmonic signals to low-loss photonic waveguides, showing potential for applications at various integration levels.

Broadband Transient Response and Wavelength-Tunable Photoacoustics in Plasmonic Hetero-nanoparticles.

The optically driven acoustic modes and nonlinear response of plasmonic nanoparticles are important in many applications, but are strongly resonant, which restricts their excitation to predefined wavelengths. Here, we demonstrate that multilayered spherical plasmonic hetero-nanoparticles, formed by alternating layers of gold and silica, provide a platform for a broadband nonlinear optical response from visible to near-infrared wavelengths. They also act as a tunable optomechanical system with mechanically decoupled layers in which different acoustic modes can be selectively switched on/off by tuning the excitation wavelength. These observations not only expand the knowledge about the internal structure of composite plasmonic nanoparticles but also allow for an additional degree of freedom for controlling their nonlinear optical and mechanical properties.

Carrier density tuning in CuS nanoparticles and thin films by Zn doping via ion exchange.

Copper sulphide (covellite) nanoplatelets have recently emerged as a plasmonic platform in the near-infrared with ultrafast nonlinear optical properties. Here we demonstrate that the free-carrier density in CuS, which is an order of magnitude lower than in traditional plasmonic metals, can be further tuned by chemical doping. Using ion exchange to replace Cu with an increasing content of Zn in the nanoparticles, the free-hole density can be lowered, resulting in a long-wavelength shift of the localised plasmon resonances from 1250 nm to 1750 nm. The proposed approach provides new opportunities for tuning the plasmonic response of covellite nanocrystals as well as the carrier relaxation time which decreases for lower free-carrier densities.

Nonlocality-Enabled Pulse Management in Epsilon-Near-Zero Metamaterials.

Ultrashort optical pulses are integral to probing various physical, chemical, and biological phenomena and feature in a whole host of applications, not least in data communications. Super- and subluminal pulse propagation and dispersion management (DM) are two of the greatest challenges in producing or counteracting modifications of ultrashort optical pulses when precise control over pulse characteristics is required. Progress in modern photonics toward integrated solutions and applications has intensified this need for greater control of ultrafast pulses in nanoscale dimensions. Metamaterials, with their unique ability to provide designed optical properties, offer a new avenue for temporal pulse engineering. Here an epsilon-near-zero metamaterial is employed, exhibiting strong nonlocal (spatial dispersion) effects, to temporally shape optical pulses. The authors experimentally demonstrate, over a wide bandwidth of tens of THz, the ability to switch from sub to superluminal and further to "backward" pulse propagation (±c/20) in the same metamaterial device by simply controlling the angle of illumination. Both the amplitude and phase of a 10 ps pulse can be controlled through DM in this subwavelength device. Shaping ultrashort optical pulses with metamaterials promises to be advantageous in laser physics, optical communications, imaging, and spectroscopy applications using both integrated and free-standing devices.

Photoelectrochemical Detection of Calcium Ions Based on Hematite Nanorod Sensors.

α-Fe2O3 (hematite) thin films have been shown to be a robust sensor substrate for photoelectrochemical imaging with good stability and high spatial resolution. Herein, one-dimensional (1D) hematite nanorods (NRs) synthesized via a simple hydrothermal method are proposed as a substrate which provides nanostructured surfaces with enhanced photocurrent responses compared to previously described hematite films, good stability, and excellent spatial resolution for potential imaging applications. The photoelectrochemical sensing capability of hematite NRs was demonstrated by a high pH sensitivity without modification. The modification of the hematite NRs with a thin poly(vinyl chloride) (PVC)-based ion-selective film allowed highly reversible amperometric detection of calcium ions with sensor materials traditionally employed in potentiometric devices.

Stable optical lateral forces from inhomogeneities of the spin angular momentum.

Transverse spin momentum related to the spin angular momentum (SAM) of light has been theoretically studied recently and predicted to generate an intriguing optical lateral force (OLF). Despite extensive studies, there is no direct experimental evidence of a stable OLF resulting from the dominant SAM rather than the ubiquitous spin-orbit interaction in a single light beam. Here, we theoretically unveil the nontrivial physics of SAM-correlated OLF, showing that the SAM is a dominant factor for the OLF on a nonabsorbing particle, while an additional force from the canonical (orbital) momentum is exhibited on an absorbing particle due to the spin-orbit interaction. Experimental results demonstrate the bidirectional movement of 5-µm-diameter particles on both sides of the beam with opposite spin momenta. The amplitude and sign of this force strongly depend on the polarization. Our optofluidic platform advances the exploitation of exotic forces in systems with a dominant SAM, facilitating the exploration of fascinating light-matter interactions.

Molecular Plasmonics with Metamaterials.

Molecular plasmonics, the area which deals with the interactions between surface plasmons and molecules, has received enormous interest in fundamental research and found numerous technological applications. Plasmonic metamaterials, which offer rich opportunities to control the light intensity, field polarization, and local density of electromagnetic states on subwavelength scales, provide a versatile platform to enhance and tune light-molecule interactions. A variety of applications, including spontaneous emission enhancement, optical modulation, optical sensing, and photoactuated nanochemistry, have been reported by exploiting molecular interactions with plasmonic metamaterials. In this paper, we provide a comprehensive overview of the developments of molecular plasmonics with metamaterials. After a brief introduction to the optical properties of plasmonic metamaterials and relevant fabrication approaches, we discuss light-molecule interactions in plasmonic metamaterials in both weak and strong coupling regimes. We then highlight the exploitation of molecules in metamaterials for applications ranging from emission control and optical modulation to optical sensing. The role of hot carriers generated in metamaterials for nanochemistry is also discussed. Perspectives on the future development of molecular plasmonics with metamaterials conclude the review. The use of molecules in combination with designer metamaterials provides a rich playground both to actively control metamaterials using molecular interactions and, in turn, to use metamaterials to control molecular processes.

Atomically Smooth Single-Crystalline Platform for Low-Loss Plasmonic Nanocavities.

Nanoparticle-on-mirror plasmonic nanocavities, capable of extreme optical confinement and enhancement, have triggered state-of-the-art progress in nanophotonics and development of applications in enhanced spectroscopies. However, the optical quality factor and thus performance of these nanoconstructs are undermined by the granular polycrystalline metal films (especially when they are optically thin) used as a mirror. Here, we report an atomically smooth single-crystalline platform for low-loss nanocavities using chemically synthesized gold microflakes as a mirror. Nanocavities constructed using gold nanorods on such microflakes exhibit a rich structure of plasmonic modes, which are highly sensitive to the thickness of optically thin (down to ∼15 nm) microflakes. The microflakes endow nanocavities with significantly improved quality factor (∼2 times) and scattering intensity (∼3 times) compared with their counterparts based on deposited films. The developed low-loss nanocavities further allow for the integration with a mature platform of fiber optics, opening opportunities for realizing nanocavity-based miniaturized photonic devices for practical applications.

Plasmonic Nanocavity Induced Coupling and Boost of Dark Excitons in Monolayer WSe2 at Room Temperature.

Spin-forbidden excitons in monolayer transition metal dichalcogenides are optically inactive at room temperature. Probing and manipulating these dark excitons are essential for understanding exciton spin relaxation and valley coherence of these 2D materials. Here, we show that the coupling of dark excitons to a metal nanoparticle-on-mirror cavity leads to plasmon-induced resonant emission with the intensity comparable to that of the spin-allowed bright excitons. A three-state quantum model combined with full-wave electrodynamic calculations reveals that the radiative decay rate of the dark excitons can be enhanced by nearly 6 orders of magnitude through the Purcell effect, therefore compensating its intrinsic nature of weak radiation. Our nanocavity approach provides a useful paradigm for understanding the room-temperature dynamics of dark excitons, potentially paving the road for employing dark exciton in quantum computing and nanoscale optoelectronics.

Photonic Spin Lattices: Symmetry Constraints for Skyrmion and Meron Topologies.

Symmetry and topology govern many electronic, magnetic, and photonic phenomena in condensed matter physics and optics, resulting in counterintuitive skyrmion, meron, and other phenomena important for modern technologies. Here we demonstrate photonic spin lattices as a new topological construct governed by the spin-orbit coupling in an optical field. The symmetry of the electromagnetic field in the presence of the spin-orbit interaction may result in only two types of photonic spin lattices: either hexagonal spin-skyrmion or square spin-meron lattices. We show that these spin structures correspond to the lowest energy of the electromagnetic field configuration, therefore, energetically stable. We further show that in the absence of spin-orbit coupling these spin topologies are degenerated in dynamic field skyrmions, unifying the description of electromagnetic field topologies. The results provide a new understanding of electromagnetic field topology and its transformations as well as new opportunities for applications in quantum technologies, spin optics, and topological photonics.

Long-Range Directional Routing and Spatial Selection of High-Spin-Purity Valley Trion Emission in Monolayer WS2.

Valley-dependent excitation and emission in transition metal dichalcogenides (TMDCs) have recently emerged as a new avenue for optical data manipulation, quantum optical technologies, and chiral photonics. The valley-polarized electronic states can be optically addressed through photonic spin-orbit interaction of excitonic emission, typically with plasmonic nanostructures, but their performance is limited by the low quantum yield of neutral excitons in TMDC multilayers and the large Ohmic loss of plasmonic systems. Here, we demonstrate a valleytronic system based on the trion emission in high-quantum-yield WS2 monolayers chirally coupled to a low-loss microfiber. The integrated system uses the spin properties of the waveguided modes to achieve long-range directional routing of valley excitations and also provides an approach to selectively address valley-dependent emission from different spatial locations around the microfiber. This valleytronic interface can be integrated with fiber communication devices, allowing for merging valley polarization and chiral photonics as an alternative mechanism for optical information transport and manipulation in classical and quantum regimes.

Ultrafast Carrier and Lattice Dynamics in Plasmonic Nanocrystalline Copper Sulfide Films.

Excited carrier dynamics in plasmonic nanostructures determines many important optical properties such as nonlinear optical response and photocatalytic activity. Here it is shown that mesoscopic plasmonic covellite nanocrystals with low free-carrier concentration exhibit a much faster carrier relaxation than in traditional plasmonic materials. A nonequilibrium hot-carrier population thermalizes within first 20 fs after photoexcitation. A decreased thermalization time in nanocrystals compared to a bulk covellite is consistent with the reduced Coulomb screening in ultrathin films. The subsequent relaxation of thermalized, equilibrium electron gas is faster than in traditional plasmonic metals due to the lower carrier concentration and agrees well with that in a bulk covellite showing no evidence of quantum confinement or hot-hole trapping at the surface states. The excitation of coherent optical phonon modes in a covellite is also demonstrated, revealing coherent lattice dynamics in plasmonic materials, which until now was mainly limited to dielectrics, semiconductors, and semimetals. These findings show advantages of this new mesoscopic plasmonic material for active control of optical processes.

Light-induced symmetry breaking for enhancing second-harmonic generation from an ultrathin plasmonic nanocavity.

Efficient frequency up-conversion of coherent light at the nanoscale is highly demanded for a variety of modern photonic applications, but it remains challenging in nanophotonics. Surface second-order nonlinearity of noble metals can be significantly boosted up by plasmon-induced field enhancement, however the related far-field second-harmonic generation (SHG) may also be quenched in highly symmetric plasmonic nanostructures despite huge near-field amplification. Here, we demonstrate that the SHG from a single gold nanosphere is significantly enhanced when tightly coupled to a metal film, even in the absence of a plasmon resonance at the SH frequency. The light-induced electromagnetic asymmetry in the nanogap junction efficiently suppresses the cancelling of locally generated SHG fields and the SH emission is further amplified through preferential coupling to the bright, bonding dipolar resonance mode of the nanocavity. The far-field SHG conversion efficiency of up to [Formula: see text] W-1 is demonstrated from a single gold nanosphere of 100 nm diameter, two orders of magnitude higher than for complex double-resonant plasmonic nanostructures. Such highly efficient SHG from a metal nanocavity also constitutes an ultrasensitive nonlinear nanoprobe to map the distribution of longitudinal vectorial light fields in nanophotonic systems.

Rapid detection of SARS-CoV-2 viral nucleic acids based on surface enhanced infrared absorption spectroscopy.

Efficient point-of-care diagnosis of severe acute respiratory syndrome-corovavirus-2 (SARS-CoV-2) is crucial for the early control of novel coronavirus infections. At present, polymerase chain reaction (PCR) is primarily used to detect SARS-CoV-2. Despite the high sensitivity, the PCR process is time-consuming and complex which limits its applicability for rapid testing of large-scale outbreaks. Here, we propose a rapid and easy-to-implement approach for SARS-CoV-2 detection based on surface enhanced infrared absorption (SEIRA) spectroscopy. The evaporated gold nano-island films are used as SEIRA substrates which are functionalized with the single-stranded DNA probes for specific binding to selected SARS-CoV-2 genomic sequences. The infrared absorption spectra are analyzed using the principal component analysis method to identify the key characteristic differences between infected and control samples. The SEIRA-based biosensor demonstrates rapid detection of SARS-CoV-2, completing the detection of 1 µM viral nucleic acids within less than 5 min without any amplification. When combined with the recombinase polymerase amplification treatment, the detection capability of 2.98 copies per µL (5 aM) can be completed within 30 min. This approach provides a simple and economical alternative for COVID-19 diagnosis, which can be potentially useful in monitoring and controlling future pandemics in a timely manner.