ACS Photonics

Harmonic and Subharmonic RF Injection Locking of THz Metasurface Quantum-Cascade VECSEL
Wu Y, Schreiber MA, Kim AD, Addamane SJ, Jirauschek C and Williams BS
Harmonic and subharmonic RF injection locking is demonstrated in a terahertz (THz) quantum-cascade vertical-external-cavity surface-emitting laser (QC-VECSEL). By tuning the RF injection frequency around integer multiples and submultiples of the cavity round-trip frequency, different harmonic and subharmonic orders can be excited in the same device. Modulation-dependent behavior of the device has been studied with recorded lasing spectral broadening and locking bandwidths in each case. In particular, harmonic injection locking results in the observation of harmonic spectra with bandwidths over 200 GHz. A semiclassical Maxwell-density matrix formalism has been applied to interpret QC-VECSEL dynamics, which aligns well with experimental observations.
Reconfigurable Integrated Thermo-Optics for Aberration Correction
Panadés JM, Rutz N, Robert HML, Steffen RT, García-Guirado J, Tessier G, Quidant R and Berto P
As miniaturization becomes a growing trend in optical systems, the ability to precisely manipulate wavefronts within micrometric pupils becomes crucial. Extensive efforts to develop integrated micro-optics primarily led to tunable microlenses. Among these approaches, , which use predesigned microheaters to locally change the refractive index in a transparent thermo-optical material, allow to produce tunable micro-optics with free-form shape. However, the shape and sign of the generated wavefront profile are fixed, predetermined by the geometry of the resistor, which severely limits its use, e.g., for aberration correction. Here, we report a precise reconfigurability of the generated wavefront through dynamic shaping of the temperature distribution, enabled by an independent control of concentric resistors. As a proof of principle, we demonstrate a bimodal that simultaneously acts as a converging/diverging lens and a positive/negative spherical aberration corrector. Through independent control of Zernike modes, this approach paves the way for compact, broadband, transparent and polarization-insensitive wavefront shapers, with a broad range of potential applications, from endoscopy to information technology.
Nanocavities for Molecular Optomechanics: Their Fundamental Description and Applications
Roelli P, Hu H, Verhagen E, Reich S and Galland C
Vibrational Raman scattering-a process where light exchanges energy with a molecular vibration through inelastic scattering-is most fundamentally described in a quantum framework where both light and vibration are quantized. When the Raman scatterer is embedded inside a plasmonic nanocavity, as in some sufficiently controlled implementations of surface-enhanced Raman scattering (SERS), the coupled system realizes an optomechanical cavity where coherent and parametrically amplified light-vibration interaction becomes a resource for vibrational state engineering and nanoscale nonlinear optics. The purpose of this Perspective is to clarify the connection between the languages and parameters used in the fields of molecular cavity optomechanics (McOM) versus its conventional, "macroscopic" counterpart and to summarize the main results achieved so far in McOM and the most pressing experimental and theoretical challenges. We aim to make the theoretical framework of molecular cavity optomechanics practically usable for the SERS and nanoplasmonics community at large. While quality factors () and mode volumes () essentially describe the performance of a nanocavity in enhancing light-matter interaction, we point to the light-cavity coupling efficiencies (η) and optomechanical cooperativities () as the key parameters for molecular optomechanics. As an illustration of the significance of these quantities, we investigate the feasibility of observing optomechanically induced transparency with a molecular vibration-a measurement that would allow for a direct estimate of the optomechanical cooperativity.
Subpicosecond Spectroscopic Ellipsometry of the Photoinduced Phase Transition in VO Thin Films
Gutiérrez Y, Vázquez-Miranda S, Espinoza S, Khakurel K, Rebarz M, Zhang Z, Saiz JM, Ramanathan S and Cueff S
We report the first application of broadband time-resolved pump-probe ellipsometry to study the ultrafast dynamics of the photoinduced insulator-to-metal transition (IMT) in vanadium dioxide (VO) thin films driven by 35 fs laser pulses. This novel technique enables the direct measurement of the time-resolved evolution of the complex pseudodielectric function of VO during the IMT. We have identified distinct thermal and nonthermal dynamics in the photoinduced IMT, which critically depends on the pump wavelength and fluence, while providing a detailed temporal and spectral phase map. A comparison of the pseudodielectric function of the VO thin film during thermally and photoinduced phase transitions reveals that the primary differences in the IMT pathways occur within the first picosecond after the pump, driven by nonequilibrium dynamics in this ultrafast time scale. The ultrafast spectroscopic ellipsometry introduced in this work offers a complementary probe to study phase changes in condensed matter and emerging photonic device materials.
Low-Power Threshold Optical Bistability Enabled by Hydrodynamic Kerr Nonlinearity of Free Carriers in Heavily Doped Semiconductors
Hu H, Álvarez-Pérez G, Otomalo TO and Ciracì C
We develop an efficient numerical model based on the semiclassical hydrodynamic theory for studying Kerr nonlinearity in degenerate electron systems such as heavily doped semiconductors. This model provides direct access to the electromagnetic responses of the quantum nature of the plasmons in heavily doped semiconductors with complex geometries, which is nontrivial for conventional frameworks. Using this model, we demonstrate nanoscale optical bistability at an exceptionally low-power threshold of 1 mW by leveraging Kerr-type hydrodynamic nonlinearities supported by the heavily doped semiconductor's free carriers. This high nonlinearity is enabled by a strong coupling between metallic gap plasmons and longitudinal bulk plasmons in the semiconductor due to quantum pressure. These findings offer a viable approach to studying Kerr-type nonlinearity and lay the groundwork for developing efficient and ultrafast all-optical nonlinear devices.
Engineering of Impact Ionization Characteristics in GaAs/GaAsBi Multiple Quantum Well Avalanche Photodiodes
Tao X, Jin X, Gao S, Yi X, Liu Y, Rockett TBO, Bailey NJ, Harun F, Adham NA, H Tan C, Richards RD and David JPR
The presence of large bismuth (Bi) atoms has been shown to increase the spin-orbit splitting energy in bulk GaAsBi, reducing the hole ionization coefficient (β) and thereby reducing the excess noise seen in avalanche photodiodes. In this study, we show that even very thin layers of GaAsBi introduced as quantum wells (QWs) in a GaAs matrix exhibit a significant reduction of β while leaving the electron ionization coefficient, α, largely unchanged. The optical and avalanche multiplication properties of a series of GaAsBi/GaAs multiple quantum well (MQW) p-i-n structures with nominally 5 nm thick, 4.4% Bi GaAsBi QWs, varying from 5 to 63 periods and corresponding barrier widths of 101 to 4 nm were investigated. From photoluminescence, ω-2θ X-ray diffraction, and cross section transmission electron microscopy measurements, the material was found to be of high quality despite the strain introduced by the Bi in all except the samples with 54 and 63 QW periods. Photomultiplication measurements undertaken with different wavelengths showed that α in these MQW structures did not change appreciably with the number of QWs; however, β decreased significantly, especially at lower values, the noise factor, , is reduced by 58% to 3.5 at a multiplication of 10, compared to a similar thickness bulk GaAs structure without any Bi. This result suggests that Bi-containing QWs could be introduced into the avalanching regions of APDs as a way of reducing their excess noise.
Nanosecond Carrier Lifetime of Hexagonal Ge
van Lange VT, Dijkstra A, Fadaly EMT, Peeters WHJ, van Tilburg MAJ, Bakkers EPAM, Bechstedt F, Finley JJ and Haverkort JEM
Hexagonal Si Ge with suitable alloy composition promises to become a new silicon compatible direct bandgap family of semiconductors. Theoretical calculations, however, predict that the binary end point of this family, the bulk hex-Ge crystal, is only weakly dipole active. This is in contrast to hex-Si Ge , where translation symmetry is broken by alloy disorder, permitting efficient light emission. Surprisingly, we observe equally strong radiative recombination in hex-Ge as in hex-Si Ge nanowires, but scrutinizing experiments on the radiative lifetime and the optical transition matrix element of hex-Ge remain hitherto unexplored. Here, we report an advanced spectral line shape analysis exploiting the Lasher-Stern-Würfel (LSW) model on an excitation density series of hex-Ge nanowire photoluminescence spectra covering 3 orders of magnitude. The analysis was performed at low temperature where radiative recombination is dominant. We analyze the amount of photoinduced bandfilling to obtain direct access to the excited carrier density, which allows to extract a radiative lifetime of (2.1 ± 0.3) ns by equating the carrier generation and recombination rates. In addition, we leveraged the LSW model to independently extract a high oscillator strength of 10.5 ± 0.9, comparable to the oscillator strength of III/V semiconductors like GaAs or GaN, showing that the optical properties of hex-Ge nanostructures are perfectly suited for a wide range of optoelectronic device applications.
Long-Range Self-Hybridized Exciton-Polaritons in Two-Dimensional Ruddlesden-Popper Perovskites
Black M, Asadi M, Darman P, Seçkin S, Schillmöller F, König TAF, Darbari S and Talebi N
Lead halide perovskites have emerged as platforms for exciton-polaritonic studies at room temperature, thanks to their excellent photoluminescence efficiency and synthetic versatility. In this work, we find proof of strong exciton-photon coupling in cavities formed by the layered crystals themselves, a phenomenon known as the self-hybridization effect. We use multilayers of high-quality Ruddlesden-Popper perovskites in their 2D crystalline form, benefiting from their quantum-well excitonic resonances and the strong Fabry-Pérot cavity modes resulting from the total internal reflection at their smooth surfaces. Optical spectroscopy reveals bending of the cavity modes typical for exciton-polariton formation, and absorption and photoluminescence spectroscopy shows splitting of the excitonic resonance and thickness-dependent peak positions. Strikingly, local optical excitation with energy below the excitonic resonance of the flakes in photoluminescence measurements unveils the coupling of light to in-plane polaritonic modes with directed propagation. These exciton-polaritons exhibit high coupling efficiencies and extremely low loss propagation mechanisms, which are confirmed by finite difference time domain simulations. Thus, we prove that mesoscopic 2D Ruddlesden-Popper perovskite flakes represent an effective but simple system to study the rich physics of exciton-polaritons at room temperature.
Surface Lattice Resonance Lasers with Epitaxial InP Gain Medium
Fischer A, Severs Millard T, Xiao X, Raziman TV, Dranczewski J, Schofield RC, Schmid H, Moselund K, Sapienza R and Oulton RF
Surface lattice resonance (SLR) lasers, where the gain is supplied by a thin-film active material and the feedback comes from multiple scattering by plasmonic nanoparticles, have shown both low threshold lasing and tunability of the angular and spectral emission at room temperature. However, typically used materials such as organic dyes and QD films suffer from photodegradation, which hampers practical applications. Here, we demonstrate photostable single-mode lasing of SLR modes sustained in an epitaxial solid-state InP slab waveguide. The nanoparticle array is weakly coupled to the optical modes, which decreases the scattering losses and hence the experimental lasing threshold is as low as 94.99 ± 0.82 μJ cm pulse. The nanoparticle periodicity defines the lasing wavelength and enables tunable emission wavelengths over a 70 nm spectral range. Combining plasmonic nanoparticles with an epitaxial solid-state gain medium paves the way for large-area on-chip integrated SLR lasers for applications, including optical communication, optical computing, sensing, and LiDAR.
Superchiral Light Emerging from Bound States in the Continuum in Metasurfaces of Si Nanorod Dimers
Pura JL, Castillo López de Larrinzar B, Liang M, García-Martín A, Gómez Rivas J and Sánchez-Gil JA
Bound states in the continuum (BICs) in all-dielectric metasurfaces enhance light-matter interaction at the nanoscale due to their infinite 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.
Approaches for Positioning the Active Medium in Hybrid Nanoplasmonics. Focus on Plasmon-Assisted Photopolymerization
Chen M, Marguet S, Issa A, Jradi S, Couteau C, Fiorini-Debuisschert C, Douillard L, Soppera O, Ge D, Plain J, Zhou X, Dang C, Béal J, Kostcheev S, Déturche R, Xu T, Wei B and Bachelot R
Over the past 20 years, hybrid plasmonics for nanoemitters of light or for nanoabsorbers, based on weak or strong coupling between metallic nanocavities and active media (emissive or absorbing entities), have given rise to important research efforts. One of the main current challenges is the control of the nanoscale spatial distribution and associated symmetry of the active medium in the vicinity of the metallic nanoparticles. In this review, we first recall the main principles of weak and strong coupling by stressing the importance of controlling the spatial distribution of the active medium and present the main approaches developed for achieving this control. Nine different approaches are identified. We then focus our attention on one of them based on plasmonic photopolymerization and discuss the flexibility of this approach in terms of control of the spatial symmetry of the hybrid nanosystem metal-polymer nanoemitters and the resulting polarization dependence of the light emission. The different approaches are analyzed and compared with each other, and some future perspectives and challenges are finally discussed.
Multiple Multicolored 3D Polarization Knots Arranged along Light Propagation
Li Y, Ansari MA, Ahmed H, Wang R, Wang G, Yu Q, Zhang C, Chen S and Chen X
Polarization and color play essential roles in understanding optical phenomena and practical applications. Customized three-dimensional (3D) light fields, characterized by specific polarization and color distributions, have garnered growing interest owing to their unique optical attributes and expanded capacity for information encoding. To align with the ongoing trend of compactness and integration, it is desirable to develop lightweight optical elements that can simultaneously control polarization and color in 3D space. Although engineering longitudinally variable 3D optical structures with predesigned color and polarization information can add more degrees of freedom and additional capacity for information encoding, it has not been reported. We propose a metasurface approach to generating multiple 3D polarization knots along the light propagation direction. Each knot features two colors and an engineered 3D polarization profile. Different multicolored 3D polarization knots are obtained by controlling the observation region along the light propagation. Our approach simultaneously combines polarization, color, and longitudinal control in 3D environment, offering extra degrees of freedom for engineering complex vector beams. The unique properties of the developed metadevices, together with the design flexibility and compactness of metasurface, pave the way for polarization systems with small volumes applicable to some areas such as complex structured beams and encryption.
Locally Phase-Engineered MoTe for Near-Infrared Photodetectors
Hidding J, Cordero-Silis CA, Vaquero D, Rompotis KP, Quereda J and Guimarães MHD
Transition-metal dichalcogenides (TMDs) are ideal systems for two-dimensional (2D) optoelectronic applications owing to their strong light-matter interaction and various band gap energies. New techniques to modify the crystallographic phase of TMDs have recently been discovered, allowing the creation of lateral heterostructures and the design of all-2D circuitry. Thus, far, the potential benefits of phase-engineered TMD devices for optoelectronic applications are still largely unexplored. The dominant mechanisms involved in photocurrent generation in these systems remain unclear, hindering further development of new all-2D optoelectronic devices. Here, we fabricate locally phase-engineered MoTe optoelectronic devices, creating a metal (1T') semiconductor (2H) lateral junction and unveil the main mechanisms at play for photocurrent generation. We find that the photocurrent originates from the 1T'-2H junction, with a maximum at the 2H MoTe side of the junction. This observation, together with the nonlinear IV-curve, indicates that the photovoltaic effect plays a major role in the photon-to-charge current conversion in these systems. Additionally, the 1T'-2H MoTe heterojunction device exhibits a fast optoelectronic response over a wavelength range of 700-1100 nm, with a rise and fall times of 113 and 110 μs, respectively, 2 orders of magnitude faster when compared to a directly contacted 2H MoTe device. These results show the potential of local phase-engineering for all-2D optoelectronic circuitry.
Study of Time-Resolved Dynamics in Turbid Medium Using a Single-Cavity Dual-Comb Laser
Zhang B, Phillips C, Venialgo Araujo E, Iskander-Rizk S, Pupeikis J, Willenberg B, Keller U and Bhattacharya N
In measuring cerebral blood flow (CBF) noninvasively using optical techniques, diffusing-wave spectroscopy is often combined with near-infrared spectroscopy to obtain a reliable blood flow index. Measuring the blood flow index at a determined depth remains the ultimate goal. In this study, we present a simple approach using dual-comb lasers where we simultaneously measure the absorption coefficient (μ), the reduced scattering coefficient (μ ), and dynamic properties. This system can also effectively differentiate dynamics from various depths, which is crucial for analyzing multilayer dynamics. For CBF measurements, this capability is particularly valuable as it helps mitigate the influence of the scalp and skull, thereby enhancing the specificity of deep tissue.
Understanding the Potential of Light Absorption in Dots-in-Host Semiconductors
Alexandre M, Águas H, Fortunato E, Martins R and Mendes MJ
The outstanding physical properties of dots-in-host (QD@Host) hetero semiconductors demand detailed methods to fundamentally understand the best routes to optimize their potentialities for different applications. In this work, a 4-band k.p-based method was developed for rock-salt quantum dots (QDs) that describes the complete optical properties of arbitrary QD@Host systems, trailblazing the way for the full optoelectronic analysis of quantum-structured solar cells. Starting with the determination of the QD bandgap and validation against well-established literature results, the electron transition rate is then computed and analyzed against the main system parameters. This is followed by a multiparameter optimization, considering intermediate band solar cells as a promising application, where the best QD configuration was determined, together with the corresponding QD@Host absorption spectrum, in view of attaining the theoretical maximum efficiency (∼50%) of this photovoltaic technology. The results show the creation of pronounced sub-bandgap absorption due to the electronic transitions from/to the quantum-confined states, which enables a much broader exploitation of the sunlight spectrum.
Extraction of Attenuation and Backscattering Coefficient along Hollow-Core Fiber Length Using Two-Way Optical Time Domain Backscattering
Wei X, Numkam Fokoua E, Poletti F and Slavík R
Optical time domain reflectometry (OTDR) is a key technique to characterize fabricated and installed optical fibers. It is also widely used in distributed sensing. OTDR of emerging hollow-core fibers (HCFs) has been demonstrated only very recently, being almost 30 dB weaker than that in the glass-core optical fibers. However, it has been challenging to extract useful data from the OTDR traces of HCFs, as the longitudinal variation in the fiber's geometry, notably the core size or the longitudinal variations of the air pressure within the core, results in commensurate changes of the backscattering strength. This is, however, necessary for continuous improvement of HCF fabrication and subsequent improvement in their performance such as minimum achievable loss, potentially enabling the use of HCF in a significantly broader range of applications than used today. Here, we demonstrate, for the first time, that the distributed loss and backscattering coefficient in antiresonant HCFs can be separated, obtaining key data about fiber distributed loss and uniformity. This is enabled by using OTDR traces obtained from both ends of the HCF.
Bound States in the Continuum and Long-Range Coupling of Polaritons in Hexagonal Boron Nitride Nanoresonators
Gupta H, Venturi G, Contino T, Janzen E, Edgar JH, De Angelis F, Toma A, Ambrosio A and Tamagnone M
Bound states in the continuum (BICs) garnered significant interest for their potential to create new types of nanophotonic devices. Most prior demonstrations were based on arrays of dielectric resonators, which cannot be miniaturized beyond the diffraction limit, reducing the applicability of BICs for advanced functions. Here, we demonstrate BICs and quasi-BICs based on high-quality factor phonon-polariton resonances in isotopically pure hBN and how these states can be supported by periodic arrays of nanoresonators with sizes much smaller than the wavelength. We theoretically illustrate how BICs emerge from the band structure of the arrays and verify both numerically and experimentally the presence of these states and enhanced quality factors. Furthermore, we identify and characterize simultaneously quasi-BICs and bright states. Our method can be generalized to create a large number of optical states and to tune their coupling with the environment, paving the way to miniaturized nanophotonic devices with more advanced functions.
Programmable Optical Synaptic Linking of Neuromorphic Photonic-Electronic RTD Spiking Circuits
Hejda M, Zhang W, Al-Taai QRA, Malysheva E, Owen-Newns D, Figueiredo JML, Romeira B, Robertson J, Dolores-Calzadilla V, Wasige E and Hurtado A
Interconnectivity between functional building blocks (such as neurons and synapses) represents a fundamental functionality for realizing neuromorphic systems. However, in the domain of neuromorphic photonics, synaptic interlinking and cascadability of spiking optical artificial neurons remains challenging and mostly unexplored in experiments. In this work, we report an optical synaptic link between optoelectronic spiking artificial neurons based upon resonant tunneling diodes (RTDs) that allows for cascadable spike propagation. First, deterministic spiking is triggered using multimodal (electrical and optical) inputs in RTD-based spiking artificial neurons, which are optoelectronic (OE) circuits incorporating either micron-scale RTDs or photosensitive nanopillar-based RTDs. Second, feedforward linking with dynamical weighting of optical spiking signals between pre- and postsynaptic RTD artificial neurons is demonstrated, including cascaded spike activation. By dynamically weighting the amplitude of optical spikes, it is shown how the cascaded spike activation probability in the postsynaptic RTD node directly follows the amplitude of the weighted optical spikes. This work therefore provides the first experimental demonstration of programmable synaptic optical link and spike cascading between multiple fast and efficient RTD OE spiking artificial neurons, therefore providing a key functionality for photonic-electronic spiking neural networks and light-enabled neuromorphic hardware.
Circularly Polarized High-Harmonic Beams Carrying Self-Torque or Time-Dependent Orbital Angular Momentum
de Las Heras A, San Román J, Serrano J, Plaja L and Hernández-García C
In the rapidly evolving field of structured light, self-torque has been recently defined as an intrinsic property of light beams carrying time-dependent orbital angular momentum. In particular, extreme-ultraviolet (EUV) beams with self-torque, exhibiting a topological charge that continuously varies on the subfemtosecond time scale, are naturally produced in high-order harmonic generation (HHG) when driven by two time-delayed intense infrared vortex beams with different topological charges. Until now, the polarization state of such EUV beams carrying self-torque has been restricted to linear states due to the drastic reduction in the harmonic up-conversion efficiency with increasing the ellipticity of the driving field. In this work, we theoretically demonstrate how to control the polarization state of EUV beams carrying self-torque, from linear to circular. The extremely high sensitivity of HHG to the properties of the driving beam allows us to propose two different driving schemes to circumvent the current limitations to manipulate the polarization state of EUV beams with self-torque. Our advanced numerical simulations are complemented with the derivation of selection rules of angular momentum conservation, which enable precise tunability over the angular momentum properties of the harmonics with self-torque. The resulting high-order harmonic emission, carrying time-dependent orbital angular momentum with a custom polarization state, can expand the applications of ultrafast light-matter interactions, particularly in areas where dichroic or chiral properties are crucial, such as magnetic materials or chiral molecules.
Deep Mouse Brain Two-Photon Near-Infrared Fluorescence Imaging Using a Superconducting Nanowire Single-Photon Detector Array
Tamimi A, Caldarola M, Hambura S, Boffi JC, Noordzij N, Los JWN, Guardiani A, Kooiman H, Wang L, Kieser C, Braun F, Castaneda MAU, Fognini A and Prevedel R
Two-photon microscopy (2PM) has become an important tool in biology to study the structure and function of intact tissues . However, adult mammalian tissues such as the mouse brain are highly scattering, thereby putting fundamental limits on the achievable imaging depth, which typically reside at around 600-800 μm. In principle, shifting both the excitation as well as (fluorescence) emission light to the shortwave near-infrared (SWIR, 1000-1700 nm) region promises substantially deeper imaging in 2PM, yet this shift has proven challenging in the past due to the limited availability of detectors and probes in this wavelength region. To overcome these limitations and fully capitalize on the SWIR region, in this work, we introduce a novel array of superconducting nanowire single-photon detectors (SNSPDs) and associated custom detection electronics for use in near-infrared 2PM. The SNSPD array exhibits high efficiency and dynamic range as well as low dark-count rates over a wide wavelength range. Additionally, the electronics and software permit a seamless integration into typical 2PM systems. Together with an organic fluorescent dye emitting at 1105 nm, we report imaging depth of >1.1 mm in the in vivo mouse brain, limited mostly by available labeling density and laser properties. Our work establishes a promising, and ultimately scalable, new detector technology for SWIR 2PM that facilitates deep tissue biological imaging.
Surpassing the Diffraction Limit in Label-Free Optical Microscopy
Palounek D, Vala M, Bujak Ł, Kopal I, Jiříková K, Shaidiuk Y and Piliarik M
Super-resolution optical microscopy has enhanced our ability to visualize biological structures on the nanoscale. Fluorescence-based techniques are today irreplaceable in exploring the structure and dynamics of biological matter with high specificity and resolution. However, the fluorescence labeling concept narrows the range of observed interactions and fundamentally limits the spatiotemporal resolution. In contrast, emerging label-free imaging methods are not inherently limited by speed and have the potential to capture the entirety of complex biological processes and dynamics. While pushing a complex unlabeled microscopy image beyond the diffraction limit to single-molecule resolution and capturing dynamic processes at biomolecular time scales is widely regarded as unachievable, recent experimental strides suggest that elements of this vision might be already in place. These techniques derive signals directly from the sample using inherent optical phenomena, such as elastic and inelastic scattering, thereby enabling the measurement of additional properties, such as molecular mass, orientation, or chemical composition. This perspective aims to identify the cornerstones of future label-free super-resolution imaging techniques, discuss their practical applications and theoretical challenges, and explore directions that promise to enhance our understanding of complex biological systems through innovative optical advancements. Drawing on both traditional and emerging techniques, label-free super-resolution microscopy is evolving to offer detailed and dynamic imaging of living cells, surpassing the capabilities of conventional methods for visualizing biological complexities without the use of labels.