Light-matter Interaction Research Articles

Reviewing advances in nanophotonic biosensors.

Biosensing, a promising branch of exploiting nanophotonic devices, enables meticulous detection of subwavelength light, which helps to analyze and manipulate light-matter interaction. The improved sensitivity of recent high-quality nanophotonic biosensors has enabled enhanced bioanalytical precision in detection. Considering the potential of nanophotonics in biosensing, this article summarizes recent advances in fabricating nanophotonic and optical biosensors, focusing on their sensing function and capacity. We typically classify these types of biosensors into five categories: phase-driven, resonant dielectric nanostructures, plasmonic nanostructures, surface-enhanced spectroscopies, and evanescent-field, and review the importance of enhancing sensor performance and efficacy by addressing some major concerns in nanophotonic biosensing, such as overcoming the difficulties in controlling biological specimens and lowering their costs for ease of access. We also address the possibility of updating these technologies for immediate implementation and their impact on enhancing safety and health.

Light funneling into localized acoustic graphene plasmons for extreme infrared and terahertz field enhancement and confinement

Enhancing light-matter interaction through deep subwavelength-scale confinement is crucial for numerous applications like molecular sensing, optoelectronic devices, and non-linear optics. Here, we report the excitation of localized acoustic graphene plasmons (LAGPs) confined in a sub-micro- wide, nanometer-thick layer using a metal slit antenna. This approach enables light funneling in the infrared and terahertz regimes, leading to strong field enhancement and confinement. LAGPs exhibit broad-band excitation characteristics, with the number of excited modes adjustable via the symmetry of the relative positioning between graphene and the metal slit. Detailed analysis indicates that the local field intensities of LAGPs are critically influenced by both the periodicity of the device structure and the electron relaxation time of graphene. These findings are effectively elucidated using temporal coupled mode theory. In comparison to conventional non-localized acoustic graphene plasmons, LAGPs demonstrate significantly improved field confinement and enhancement attributed to the funneling effect. Our study presents a promising avenue for achieving robust light-matter interaction and holds potential for various applications in the infrared and terahertz domains.

Optical atompilz: Propagation-invariant strongly longitudinally polarized toroidal pulses

Recent advancements in optical, terahertz, and microwave systems have unveiled non-transverse optical toroidal pulses characterized by skyrmionic topologies, fractal-like singularities, space-time nonseparability, and anapole-exciting ability. Despite this, the longitudinally polarized fields of canonical toroidal pulses notably lag behind their transverse counterparts in magnitude. Interestingly, although mushroom-cloud-like toroidal vortices with strong longitudinal fields are common in nature, they remain unexplored in the realm of electromagnetics. Here, we present strongly longitudinally polarized toroidal pulses (SLPTPs), which boast a longitudinal component amplitude exceeding that of the transverse component by over tenfold. This unique polarization property endows SLPTPs with robust propagation characteristics, showcasing nondiffracting behavior. The propagation-invariant strongly longitudinally polarized field holds promise for pioneering light–matter interactions, far-field superresolution microscopy, and high-capacity wireless communication utilizing three polarizations.

Spatiotemporal hologram

Spatiotemporal structured light has opened up new avenues for optics and photonics. Current spatiotemporal manipulation of light mostly relies on phase-only devices such as liquid crystal spatial light modulators to generate spatiotemporal optical fields with unique photonic properties. However, simultaneous manipulation of both amplitude and phase of the complex field for the spatiotemporal light is still lacking, limiting the diversity and richness of achievable photonic properties. In this work, a simple and versatile spatiotemporal holographic method that can arbitrarily sculpt the spatiotemporal light is presented. The capabilities of this simple yet powerful method are demonstrated through the generation of fundamental and higher-order spatiotemporal Bessel wavepackets, spatiotemporal crystal-like and quasi-crystal-like structures, and spatiotemporal flat-top wavepackets. Fully customizable spatiotemporal wavepackets will find broader application in investigating the dynamics of spatiotemporal fields and interactions between ultrafast spatiotemporal pulses and matters, unveiling previously hidden light-matter interactions and unlocking breakthroughs in photonics and beyond.

Distributed semiconductor heterojunctions of ZnO–Cu2O for ultraviolet photodetection

Semiconductor heterojunctions, because of their unique optoelectronic properties, have gained significant attention for integrated photonic devices. UV photodetectors based on semiconductor heterojunctions are promising due to their enhanced light absorption, efficient charge separation, and tunable electronic properties, which collectively lead to superior sensitivity and performance. An inter-band transition-based UV photodetector utilizing Cu2O/ZnO distributed heterojunctions has been demonstrated. We propose an integrated photonic structure based on semiconductor heterojunctions in the form of Cu2O–ZnO grating for ultraviolet photodetection yielding a low dark current and improved efficiency. The Cu2O–ZnO grating heterostructure, in comparison to individual planar heterojunction, boosts light-matter interaction enabling higher absorption and enhanced responsivity. The device depicts a responsivity of 0.7A/W at 360nm wavelength. The device exhibits a broadband absorption which remains good over a broad wavelength range from 250nm to 450nm. The reported UV photodetector may find applications in environmental monitoring, UV light communication, biomedical diagnostics, and industrial safety.

Terahertz characterization of organic crystals using paraffin as dilution matrix

Terahertz waves exhibit excellent performance in molecular information detection of substances. Since natural materials exhibit weak absorption of terahertz waves, it's conventional to involve mixing analyte with polymer diluents and pressing them into pellets, or enhance the light-material interaction through coupling systems of natural materials with metamaterials. However, both pressure-induced metastable crystal structure transformations and spatial overlap between the analyte and metasurfaces can impact the absorption of terahertz waves by organic crystals. This paper proposes a novel analytical approach using paraffin as a dilution matrix for qualitatively and quantitatively characterizing organic crystals with THz spectroscopy. The featureless refractive index spectra and negligible absorption demonstrated the feasibility of paraffin as a diluting analyte. The analytical process was further demonstrated with well-studied lactose by being diluted in molten paraffin at different mass-ratios and solidified as pellets under room temperature and ambient pressure. A continuous wave terahertz frequency domain spectroscopy system (THz-FDS) is used for spectral acquisition over 0.4–1.3 THz. The experimental results reveal a significant linear correlation between the absorption coefficient peak areas and molar concentration of lactose, with a correlation coefficient R2 of 0.9678. Our method provides an additional optional dilution matrix for terahertz spectroscopy characterization of organic crystals, enabling non-destructive, rapid, and direct measurement of metastable crystals. Furthermore, this study on paraffin as a binder material holds potential for enhancing spatial overlap between natural materials and metamaterials in the field of metasurface-enhanced sensing.

Recent Progress in the Synthesis of 3D Complex Plasmonic Intragap Nanostructures and Their Applications in Surface-Enhanced Raman Scattering.

Plasmonic intragap nanostructures (PINs) have garnered intensive attention in Raman-related analysis due to their exceptional ability to enhance light-matter interactions. Although diverse synthetic strategies have been employed to create these nanostructures, the emphasis has largely been on PINs with simple configurations, which often fall short in achieving effective near-field focusing. Three-dimensional (3D) complex PINs, distinguished by their intricate networks of internal gaps and voids, are emerging as superior structures for effective light trapping. These structures facilitate the generation of hot spots and hot zones that are essential for enhanced near-field focusing. Nevertheless, the synthesis techniques for these complex structures and their specific impacts on near-field focusing are not well-documented. This review discusses the recent advancements in the synthesis of 3D complex PINs and their applications in surface-enhanced Raman scattering (SERS). We begin by describing the foundational methods for fabricating simple PINs, followed by a discussion on the rational design strategies aimed at developing 3D complex PINs with superior near-field focusing capabilities. We also evaluate the SERS performance of various 3D complex PINs, emphasizing their advanced sensing capabilities. Lastly, we explore the future perspective of 3D complex PINs in SERS applications.

Stealthy and hyperuniform isotropic photonic band gap structure in 3D.

In photonic crystals, the propagation of light is governed by their photonic band structure, an ensemble of propagating states grouped into bands, separated by photonic band gaps. Due to discrete symmetries in spatially strictly periodic dielectric structures their photonic band structure is intrinsically anisotropic. However, for many applications, such as manufacturing artificial structural color materials or developing photonic computing devices, but also for the fundamental understanding of light-matter interactions, it is of major interest to seek materials with long range nonperiodic dielectric structures which allow the formation of isotropic photonic band gaps. Here, we report the first ever 3D isotropic photonic band gap for an optimized disordered stealthy hyperuniform structure for microwaves. The transmission spectra are directly compared to a diamond pattern and an amorphous structure with similar node density. The band structure is measured experimentally for all three microwave structures, manufactured by 3D laser printing for metamaterials with refractive index up to . Results agree well with finite-difference-time-domain numerical investigations and a priori calculations of the band gap for the hyperuniform structure: the diamond structure shows gaps but being anisotropic as expected, the stealthy hyperuniform pattern shows an isotropic gap of very similar magnitude, while the amorphous structure does not show a gap at all. Since they are more easily manufactured, prototyping centimeter scaled microwave structures may help optimizing structures in the technologically very interesting region of infrared.

Ultrasensitive Terahertz Fingerprint Retrieval with Multiple‐BIC‐Enabled Meta‐Sensors

AbstractBound states in the continuum (BICs) are an excellent platform enabling highly efficient light–matter interaction in applications for lasing, nonlinear generation, and sensing. However, the current focus in implementing BICs has primarily been on single sharp resonances, limiting the extent of electric field enhancement for multiple resonances. In this study, experimental demonstrations are conducted to showcase how metasurfaces can enable the control of symmetry‐broken and Friedrich–Wintgen BICs by leveraging the asymmetry of split resonant rings. This approach allows for the existence of multiple free‐control BIC resonances and tailored enhancement of controlling light–matter interactions. Further experiments are conducted to validate the effectiveness and performance of meta‐sensors for the identification of the distinct fingerprint of α‐lactose with high sensitivity using only one single metasurface. These findings present a novel and efficient platform for the development of miniaturized and chip‐scale photonics devices with intense light–matter interaction.

Methods in molecular photocrystallography.

Over the last three decades, the technology that makes it possible to follow chemical processes in the solid state in real time has grown enormously. These studies have important implications for the design of new functional materials for applications in optoelectronics and sensors. Light-matter interactions are of particular importance, and photocrystallography has proved to be an important tool for studying these interactions. In this technique, the three-dimensional structures of light-activated molecules, in their excited states, are determined using single-crystal X-ray crystallography. With advances in the design of high-power lasers, pulsed LEDs and time-gated X-ray detectors, the increased availability of synchrotron facilities, and most recently, the development of XFELs, it is now possible to determine the structures of molecules with lifetimes ranging from minutes down to picoseconds, within a single crystal, using the photocrystallographic technique. This review discusses the procedures for conducting successful photocrystallographic studies and outlines the different methodologies that have been developed to study structures with specific lifetime ranges. The complexity of the methods required increases considerably as the lifetime of the excited state shortens. The discussion is supported by examples of successful photocrystallographic studies across a range of timescales and emphasises the importance of the use of complementary analytical techniques in order to understand the solid-state processes fully.

Intense pulsed light-induced millisecond selective heat treatment for high-performance silicon anodes

Silicon, which is gaining prominence as a potential anode material, exhibits long-term cycle stability issues owing to volume changes during cycling. This study presents a meticulously designed Si anode that employs intense pulsed light (IPL) technology to simultaneously reduce carbon additives and construct an effective carbon quantum dot (CQD)-derived binder system. IPL, as a light-material interaction technique, offers a novel approach for selective heat treatment with remarkably short processing durations on the order of milliseconds. By comprehensively considering the geometric structure, optical characteristics, and thermal properties of each electrode component, heat transfer bridge (HTB) materials are introduced to ensure a homogeneous depth-directional heat treatment and to minimize binder decomposition in the IPL process. By employing HTB materials, the binder can reach a controlled target temperature for the condensation reaction between poly (acrylic acid) and the CQDs. Simultaneously, higher heat generation in the conductive carbon than in the binder leads to selective additional carbon reduction. This unique approach provides selective heat treatment, which cannot be achieved using conventional methods, resulting in a Si anode with excellent cyclic stability and rate capability. The versatility of the IPL technology is further demonstrated by applying it to relatively inexpensive Si microparticles.

Dual Plasmons with Bioinspired 3D Network Structure Enabling Ultrahigh Efficient Solar Steam Generation.

Plasmonic nanomaterials such as Au, Ag, and Cu are widely recognized for their strong light-matter interactions, making them promising photothermal materials for solar steam generation. However, their practical use in water evaporation is significantly limited by the trade-off between high costs and poor stability. In this regard, we introduce a novel, nonmetallic dual plasmonic TiN/MoO3-x composite. This composite features a three-dimensional, urchin-like biomimetic structure, with plasmonic TiN nanoparticles embedded within a network of plasmonic MoO3-x nanorods. As a solar absorber, the TiN/MoO3-x composite achieves a high evaporation rate of ∼2.05 kg m-2 h-1 with an energy efficiency up to 106.7% under 1 sun illumination, outperforming the state-of-the-art plasmonic systems. The high photothermal stability and unique dual plasmonic nanostructure of the TiN/MoO3-x composite are demonstrated by advanced in situ laser-heating transmission electron microscopy and photon-induced near-field electron microscopy/electron energy-loss spectroscopy, respectively. This work provides new inspiration for the design of plasmonic materials.

Superchiral Light Emerging from Bound States in the Continuum in Metasurfaces of Si Nanorod Dimers.

Bound states in the continuum (BICs) in all-dielectric metasurfaces enhance light-matter interaction at the nanoscale due to their infinite Q factors and strong field confinement. Among a variety of phenomena already reported, their impact on chiral light has recently attracted great interest. Here we investigate the emergence of intrinsic and extrinsic optical chirality associated with the excitation of BICs in various metasurfaces made of Si nanorod dimers on a quartz substrate, comparing three cases: parallel nanorods (neutral) and shifted and slanted dimers, with/without index-matching superstrate. We analyze both the circular dichroism (CD) of the far-field (FF) interaction and the helicity of the near-field (NF) distribution. We show that the best approach to achieve chiral response in the FF based on extrinsic chirality is to exploit quasi-BICs (q-BICs) appearing in the case of slanted nanorod dimers. By contrast, the helicity density is largely enhanced in the case of shifted dimers, as it presents intrinsic chirality, with values 2 orders of magnitude larger than those of circularly polarized plane waves. These so-called superchiral electromagnetic fields concentrated at the nanoscale within the metasurface hold promise of appealing implications in phenomena such as strong-coupling, photoluminescence emission, or other local light-matter interactions.

Self-Driven Graphene Photodetector Arrays Enabled by Plasmon-Induced Asymmetric Electric Field.

Gap surface plasmon (GSP) modes enhance graphene photodetectors (GPDs)' performance by confining the incident light within nanogaps, giving rise to strong light absorption. Here, we propose an asymmetric plasmonic nanostructure array on planar graphene comprising stripe- and triangle-shaped sharp tip arrays. Upon light excitation, the noncentrosymmetric metallic nanostructures show strong light-matter interactions with localized field close to the surface of tips, causing an asymmetric electric field. These features can accelerate the hot electron generation in graphene, forming a directional diffusion current. Accordingly, the artificial GPDs exhibit a wavelength-dependence behavior covering the wavelength range from 0.8 to 1.6 μm, with three photoresponse maxima corresponding to the nanostructures' resonances. Additionally, the polarization-dependent GPDs can realize a responsivity of ∼25 mA/W and a noise equivalent power of ∼0.44 nW/Hz1/2 at zero bias when excited at the resonance of 1.4 μm. Overall, our study offers a new strategy for preparing compact and multifrequency infrared GPDs.

Enhanced Photocatalytic Properties and Photoinduced Crystallization of TiO2-Fe2O3 Inverse Opals Fabricated by Atomic Layer Deposition.

The use of solar energy for photocatalysis holds great potential for sustainable pollution reduction. Titanium dioxide (TiO2) is a benchmark material, effective under ultraviolet light but limited in visible light utilization, restricting its application in solar-driven photocatalysis. Previous studies have shown that semiconductor heterojunctions and nanostructuring can broaden the TiO2's photocatalytic spectral range. Semiconductor heterojunctions are interfaces formed between two different semiconductor materials that can be engineered. Especially, type II heterojunctions facilitate charge separation, and they can be obtained by combining TiO2 with, for example, iron(III) oxide (Fe2O3). Nanostructuring in the form of 3D inverse opals (IOs) demonstrated increased TiO2 light absorption efficiency of the material, by tailoring light-matter interactions through their photonic crystal structure and specifically their photonic stopband, which can give rise to a slow photon effect. Such effect is hypothesized to enhance the generation of free charges. This work focuses on the above-described effects simultaneously, through the synthesis of TiO2-Fe2O3 IOs via multilayer atomic layer deposition (ALD) and the characterization of their photocatalytic activities. Our results reveal that the complete functionalization of TiO2 IOs with Fe2O3 increases the photocatalytic activity through the slow photon effect and semiconductor heterojunction formation. We systematically explore the influence of Fe2O3 thickness on photocatalytic performance, and a maximum photocatalytic rate constant of 1.38 ± 0.09 h-1 is observed for a 252 nm template TiO2-Fe2O3 bilayer IO consisting of 16 nm TiO2 and 2 nm Fe2O3. Further tailoring the performance by overcoating with additional TiO2 layers enhances photoinduced crystallization and tunes photocatalytic properties. These findings highlight the potential of TiO2-Fe2O3 IOs for efficient water pollutant removal and the importance of precise nanostructuring and heterojunction engineering in advancing photocatalytic technologies.

Wafer-Scale Replication of Plasmonic Nanostructures via Microbubbles for Nanophotonics.

Quasi-3D plasmonic nanostructures are in high demand for their ability to manipulate and enhance light-matter interactions at subwavelength scales, making them promising building blocks for diverse nanophotonic devices. Despite their potential, the integration of these nanostructures with optical sensors and imaging systems on a large scale poses challenges. Here, a robust technique for the rapid, scalable, and seamless replication of quasi-3D plasmonic nanostructures is presented straight from their production wafers using a microbubble process. This approach not only simplifies the integration of quasi-3D plasmonic nanostructures into a wide range of standard and custom optical imaging devices and sensors but also significantly enhances their imaging and sensing performance beyond the limits of conventional methods. This study encompasses experimental, computational, and theoretical investigations, and it fully elucidates the operational mechanism. Additionally, it explores a versatile set of options for outfitting nanophotonic devices with custom-designed plasmonic nanostructures, thereby fulfilling specific operational criteria.

Miniaturized quasi-BICs based on a two-dimensional heterostructure to realize a low-threshold nanolaser.

Bound states in the continuum (BICs) have been demonstrated as an effective mechanism to achieve high quality (Q)-factor cavities for nanolasers. However, the development of a compact BIC laser with a low threshold has remained elusive. Here, we numerically report lasing action from symmetry-protected BICs in a two-dimensional heterostructure, which consists of compound gratings with finite cells surrounded by orthogonal distributed Bragg reflectors (DBRs). The compound grating is used to excite quasi-BIC resonance with a high Q-factor, and DBRs enable light confinement and localized electric fields to enhance light-matter interaction. The nanolaser with a threshold of 16.8 µJ/cm2 is achieved within a footprint as small as 3.35 × 3.35 µm2. By changing the phase adjusting gap or asymmetry degree, it is possible to control the lasing emission. This work reveals a new, to our knowledge, path toward compact BIC lasers with a simple scheme for applications that require a small footprint and low threshold.

Polarization-Controlled Exciton-Polaritons in WS2 Strongly Coupled with Low-Symmetry Photonic Crystal Nanostructures.

Atomically thin transition metal dichalcogenides (TMDs) with ambient stable exciton resonances have emerged as an ideal material platform for exciton-polaritons. In particular, the strong coupling between excitons in TMDs and optical resonances in anisotropic photonic nanostructures can form exciton-polaritons with polarization selectivity, which offers a new degree of freedom for the manipulation of the light-matter interaction. In this work, we present the experimental demonstration of polarization-controlled exciton-polaritons in tungsten disulfide (WS2) strongly coupled with polarization singularities in the momentum space of low-symmetry photonic crystal (PhC) nanostructures. The utilization of polarization singularities can not only effectively modulate the polarization states of exciton-polaritons in the momentum space but also facilitate or suppress their far field coupling capabilities by tuning the in-plane momentum. Our results provide new strategies for creating polarization-selective exciton-polaritons.

Light-matter interaction during and post polymerization in self-written polymer waveguide integrated with optical fibers

Self-written polymer waveguide is a polymer interconnection structure often integrated with optical fibers. The structure is fabricated by photopolymerization, through which a photon beam initiates a polymerization reaction to change liquid monomer into a solid polymer. During light-matter interaction photoinitiator molecules are excited to the singlet and then to the third state to form free radicals by attaching to the adjacent monomer molecules. The free radicals in turn form polymer chains and cross-linked structures. Photo-induced polymerization leads to a raised refractive index of the monomer and forms an optical waveguide. The change is permanent to allow the process of self-focusing and self-trapping of the propagation light beam and hence guide it to the aligned optical fiber. In this article, light matter interaction during polymer waveguide fabrication and post polymerization has been investigated. A photopolymer system of acrylate-based monomer, co-initiator amine and photo initiator is used to study the absorption of the monomer mixture at the spectral range of 450–550 nm. Then photobleaching was investigated after waveguide fabrication. The optical transmission efficiency of the polymer bridge increases as absorption ceases within the polymer structure such that optical loss reduces from 1.1 dB to about 0.65 dB.

Spatiotemporal determination of photoinduced strain in a Weyl semimetal.

The application of dynamic strain holds the potential to manipulate topological invariants in topological quantum materials. This study investigates dynamic structural deformation and strain modulation in the Weyl semimetal WTe2, focusing on the microscopic regions with static strain defects. The interplay of static strain fields, at local line defects, with dynamic strain induced from photo-excited coherent acoustic phonons results in the formation of local standing waves at the defect sites. The dynamic structural distortion is precisely determined utilizing ultrafast electron microscopy with nanometer spatial and gigahertz temporal resolutions. Numerical simulations are employed to interpret the experimental results and explain the mechanism for how the local strain fields are transiently modulated through light-matter interaction. This research provides the experimental foundation for investigating predicted phenomena such as the mixed axial-torsional anomaly, acoustogalvanic effect, and axial magnetoelectric effects in Weyl semimetals, and paves the road to manipulate quantum invariants through transient strain fields in quantum materials.