monitoring-conformational-dynamics-single-unmodified-proteins-using

Monitoring Conformational Dynamics of Single Unmodified Proteins using Plasmonic Nanotweezers

Current single-molecule techniques to characterize proteins typically require labels, tethers, or the use of non-native solution conditions. Such changes ...

Nottingham Trent University

Advance of photonics media is restrained by the lack of structuring techniques for the 3D fabrication of active materials with long-range periodicity. A methodology is reported for the engineering of tunable resonant photonic media with thickness exceeding the plasmonic near-field enhancement region by more than two orders of magnitude. The media architecture consists of a stochastically ordered distribution of plasmonic nanocrystals in a fractal scaffold of high-index semiconductors. This plasmonic-semiconductor fractal media supports the propagation of surface plasmons with drastically enhanced intensity over multiple length scales, overcoming the 2D limitations of established metasurface technologies. The fractal media are used for the fabrication of plasmonic optical gas sensors, achieving a limit of detection of 0.01 vol% at room temperature and sensitivity up to 1.9 nm vol% , demonstrating almost a fivefold increase with respect to an optimized planar geometry. Beneficially to their implementation, the self-assembly mechanism of this fractal architecture allows fabrication of micrometer-thick media over surfaces of several square centimeters in a few seconds. The designable optical features and intrinsic scalability of these photonic fractal metamaterials provide ample opportunities for applications, bridging across transformation optics, sensing, and light harvesting.

Photonic Fractal Metamaterials: A Metal-Semiconductor Platform with Enhanced Volatile-Compound Sensing Performance.

Optical force is a powerful tool to actuate micromachines. Conventional approaches often require focusing and steering an incident laser beam, resulting in a bottleneck for the integration of the optically actuated machines. Here, we propose a linear nanomotor based on a plasmonic particle that generates, even when illuminated with a plane wave, a lateral optical force due to its directional side scattering. This force direction is determined by the orientation of the nanoparticle rather than a field gradient or propagation direction of the incident light. We demonstrate the arrangements of the particles allow controlling the lateral force distributions with the resolution beyond the diffraction limit, which can produce movements, as designed, of microobjects in which they are embedded without shaping and steering the laser beam. Our nanomotor to engineer the experienced force can open the door to a new class of micro/nanomechanical devices that can be entirely operated by light.

Plasmonic linear nanomotor using lateral optical forces.

Nonlinear light sources are central to a myriad of applications, driving a quest for their miniaturisation down to the nanoscale. In this quest, nonlinear metasurfaces hold a great promise, as they enhance nonlinear effects through their resonant photonic environment and high refractive index, such as in high-index dielectric metasurfaces. However, despite the sub-diffractive operation of dielectric metasurfaces at the fundamental wave, this condition is not fulfilled for the nonlinearly generated harmonic waves, thereby all nonlinear metasurfaces to date emit multiple diffractive beams. Here, we demonstrate the enhanced single-beam second- and third-harmonic generation in a metasurface of crystalline transition-metal-dichalcogenide material, offering the highest refractive index. We show that the interplay between the resonances of the metasurface allows for tuning of the unidirectional second-harmonic radiation in forward or backward direction, not possible in any bulk nonlinear crystal. Our results open new opportunities for metasurface-based nonlinear light-sources, including nonlinear mirrors and entangled-photon generation.

Tunable unidirectional nonlinear emission from transition-metal-dichalcogenide metasurfaces.

An innovative time-varying metasurface has been reported to realise dual-channel data transmissions for light-to-microwave signal conversion. Such a novel technique is a remarkable step forward to realise full-spectrum networks for catering for the growing demand for wireless communications. Moreover, this technique enriches the functionalities of tunable metasurfaces and stimulates new information-oriented applications.

Programmable structured surfaces can change the future of wireless communications.

Resonant metasurfaces provide a unique platform for enhancing multiwave nonlinear interactions. However, the difficulties over mode matching and material transparency place significant challenges in the enhancement of these multiwave processes. Here we demonstrate efficient nonlinear sum-frequency generation (SFG) in multiresonant GaP metasurfaces based on guided-wave bound-state in the continuum resonances. The excitation of the metasurface by two near-infrared input beams generates strong SFG in the visible spectrum with a conversion efficiency of 2.5 × 10 W, 2 orders of magnitude higher than the one reported in Mie-type resonant metasurfaces. In addition, we demonstrate the nontrivial polarization dependence on the SFG process. In contrast to harmonic generation, the SFG process is enhanced when using nonparallel polarized input-beams. Importantly, by varying the input pump beam polarization it is possible to direct the SFG emission to different diffraction orders, thereby opening up new opportunities for nonlinear light sources and infrared to visible light conversion.

Sum-Frequency Generation in High-Q GaP Metasurfaces Driven by Leaky-Wave Guided Modes.

Nanopore sensors provide a unique platform to detect individual nucleic acids, proteins, and other biomolecules without the need for fluorescent labeling or chemical modifications. Solid-state nanopores offer the potential to integrate nanopore sensing with other technologies such as field-effect transistors (FETs), optics, plasmonics, and microfluidics, thereby attracting attention to the development of commercial instruments for diagnostics and healthcare applications. Stable nanopores with ideal dimensions are particularly critical for nanopore sensors to be integrated into other sensing devices and provide a high signal-to-noise ratio. Nanopore fabrication, although having benefited largely from the development of sophisticated nanofabrication techniques, remains a challenge in terms of cost, time consumption and accessibility. One of the latest developed methods-controlled breakdown (CBD)-has made the nanopore technique broadly accessible, boosting the use of nanopore sensing in both fundamental research and biomedical applications. Many works have been developed to improve the efficiency and robustness of pore formation by CBD. However, nanopores formed by traditional CBD are randomly positioned in the membrane. To expand nanopore sensing to a wider biomedical application, controlling the localization of nanopores formed by CBD is essential. This article reviews the recent strategies to control the location of nanopores formed by CBD. We discuss the fundamental mechanism and the efforts of different approaches to confine the region of nanopore formation.

Localized Nanopore Fabrication via Controlled Breakdown.

Low-cost large-area chirality meta-devices (CMDs) with adjustable optical chirality are of great interest for polarization-sensitive imaging, stereoscopic display, enantioselectivity analysis, and catalysis. Currently, CMDs with adjusted chiroptical responses in the mid-infrared to terahertz band have been demonstrated by exploiting photocarriers of silicon, pressure, and phase-change of GSTs but are still absent in the visible band, which in turn limits the development of chiral nanophotonic devices. Herein, by employing a phase-change material (SbS), we present a protocol for the fabrication of wafer-scale visible-band enantiomeric CMDs with handedness, spectral, and polarization adjustability. As measured by circular dichroism, the chirality signs of CMDs enantiomers can be adjusted with SbS from amorphous to crystalline, and the chirality resonance wavelength can also be adjusted. Our results suggest a new type of meta-devices with adjustable chiroptical responses that may potentially enable a wide range of chirality nanophotonic applications including highly sensitive sensing and surface-enhanced nanospectroscopy.

Visible-Band Chiroptical Meta-devices with Phase-Change Adjusted Optical Chirality.

In the last decades, metasurfaces have attracted much attention because of their extraordinary light-scattering properties. However, their inherently static geometry is an obstacle to many applications where dynamic tunability in their optical behaviour is required. Currently, there is a quest to enable dynamic tuning of metasurface properties, particularly with fast tuning rate, large modulation by small electrical signals, solid state and programmable across multiple pixels. Here, we demonstrate electrically tunable metasurfaces driven by thermo-optic effect and flash-heating in silicon. We show a 9-fold change in transmission by <5 V biasing voltage and the modulation rise-time of <625 µs. Our device consists of a silicon hole array metasurface encapsulated by transparent conducting oxide as a localised heater. It allows for video frame rate optical switching over multiple pixels that can be electrically programmed. Some of the advantages of the proposed tuning method compared with other methods are the possibility to apply it for modulation in the visible and near-infrared region, large modulation depth, working at transmission regime, exhibiting low optical loss, low input voltage requirement, and operating with higher than video-rate switching speed. The device is furthermore compatible with modern electronic display technologies and could be ideal for personal electronic devices such as flat displays, virtual reality holography and light detection and ranging, where fast, solid-state and transparent optical switches are required.

Electrically programmable solid-state metasurfaces via flash localised heating.

Ferritin is a protein that stores and releases iron to prevent diseases associated with iron dysregulation in plants, animals, and bacteria. The conversion between iron-loaded holo-ferritin and empty apo-ferritin is an important process for iron regulation. To date, studies of ferritin have used either ensemble measurements to quantify the characteristics of a large number of proteins or single-molecule approaches to interrogate labeled or modified proteins. Here we demonstrate the first real-time study of the dynamics of iron ion loading and biomineralization within a single, unlabeled ferritin protein. Using optical nanotweezers, we trapped single apo- and holo-ferritins indefinitely, distinguished one from the other, and monitored their structural dynamics in real time. The study presented here deepens the understanding of the iron uptake mechanism of ferritin proteins, which may lead to new therapeutics for iron-related diseases.

Optical Monitoring of  Iron Loading into Single, Native Ferritin Proteins.

Ferritin, a spherical protein shell assembled from 24 subunits, functions as an efficient iron storage and release system through its channels. Understanding how various chemicals affect the structural behavior of ferritin is crucial for unravelling the origins of iron-related diseases in living organisms including humans. In particular, the influence of chemicals on ferritin's dynamics and iron release is barely explored at the single-protein level. Here, by employing optical nanotweezers using double-nanohole (DNH) structures, we examined the effect of ascorbic acid (reducing reagent) and pH on individual ferritin's conformational dynamics. The dynamics of ferritin increased as the concentration of ascorbic acid approached saturation. At pH 2.0, ferritin exhibited significant structural fluctuations and eventually underwent a stepwise disassembly into fragments. This work demonstrated the disassembly pathway and kinetics of a single ferritin molecule in solution. We identified four critical fragments during its disassembly pathway, which are 22-mer, 12-mer, tetramer, and dimer subunits. Moreover, we present single-molecule evidence of the cooperative disassembly of ferritin. Interrogating ferritin's structural change in response to different chemicals holds importance for understanding their roles in iron metabolism, hence facilitating further development of medical treatments for its associated diseases.

Structural Flexibility and Disassembly Kinetics of Single Ferritin Molecules Using Optical Nanotweezers.

Nonlinear metasurfaces have experienced rapid growth recently due to their potential in various applications, including infrared imaging and spectroscopy. However, due to the low conversion efficiencies of metasurfaces, several strategies have been adopted to enhance their performances, including employing resonances at signal or nonlinear emission wavelengths. This strategy results in a narrow operational band of the nonlinear metasurfaces, which has bottlenecked many applications, including nonlinear holography, image encoding, and nonlinear metalenses. Here, we overcome this issue by introducing a new nonlinear imaging platform utilizing a pump beam to enhance signal conversion through four-wave mixing (FWM), whereby the metasurface is resonant at the pump wavelength rather than the signal or nonlinear emissions. As a result, we demonstrate broadband nonlinear imaging for arbitrary objects using metasurfaces. A silicon disk-on-slab metasurface is introduced with an excitable guided-mode resonance at the pump wavelength. This enabled direct conversion of a broad IR image ranging from >1000 to 4000 nm into visible. Importantly, adopting FWM substantially reduces the dependence on high-power signal inputs or resonant features at the signal beam of nonlinear imaging by utilizing the quadratic relationship between the pump beam intensity and the signal conversion efficiency. Our results, therefore, unlock the potential for broadband infrared imaging capabilities with metasurfaces, making a promising advancement for next-generation all-optical infrared imaging techniques with chip-scale photonic devices.

Broadband infrared imaging governed by guided-mode resonance in dielectric metasurfaces.

Metasurfaces, composed of artificial meta-atoms of subwavelength size, can support strong light-matter interaction based on multipolar resonances and plasmonics, hence offering the great capability of empowering nonlinear generation. Recently, owing to their ability to manipulate the amplitude and phase of the nonlinear emission in the subwavelength scale, metasurfaces have been recognized as ultra-compact, flat optical components for a vast range of applications, including nonlinear imaging, quantum light sources, and ultrasensitive sensing. This review focuses on the recent progress on nonlinear metasurfaces for those applications. The principles and advances of metasurfaces-based techniques for image generation, including image encoding, holography, and metalens, are investigated and presented. Additionally, the overview and development of spontaneous photon pair generation from metasurfaces are demonstrated and discussed, focusing on the aspects of photon pair generation rate and entanglement of photon pairs. The recent blossoming of the nonlinear metasurfaces field has triggered growing interest to explore its ability to efficiently up-convert infrared images of arbitrary objects to visible images and achieve spontaneous parametric down-conversion. This recently emerged direction holds promising potential for the next-generation technology in night-vision, quantum computing, and biosensing fields.

Advances in nonlinear metasurfaces for imaging, quantum, and sensing applications.

Symmetry-protected bound states in the continuum (SP-BICs) are one of the most intensively studied BICs. Typically, SP-BICs must be converted into quasi-BICs (QBICs) by breaking the unit cell's symmetry so that they can be accessed by the external excitation. The symmetry-broken usually results in a varied resonance wavelength of QBICs which are also highly sensitive to the asymmetry parameters. In this work, we demonstrate that QBICs with a stable resonance wavelength can be realized by breaking translational symmetry in an all-dielectric metasurface. The unit cell of metasurface is made of a silicon nanodisk dimer. The Q-factor of QBICs is precisely tuned by changing the interspacing of two nanodisks while their resonance wavelength is quite stable against the interspacing. We also find that such BICs show weak dependence on the shape of the nanodisk. Multiple decompositions indicate that the toroidal dipole dominates this type of QBIC. The resonance wavelengths of QBICs can be tuned only by changing either the lattice constants or the radius of nanodisk. Finally, we present experimental demonstrations on such a QBIC with a stable resonance wavelength. The highest measured Q-factor of QBICs is >3000. Our results may find promising applications in enhancing light-matter interaction.

Article	Year
Photonic Fractal Metamaterials: A Metal-Semiconductor Platform with Enhanced Volatile-Compound Sensing Performance. Advanced materials (Deerfield Beach, Fla.)\| PubMed ID: 33089556	2020
Plasmonic linear nanomotor using lateral optical forces. Science advances\| PubMed ID: 33148646	2020
Tunable unidirectional nonlinear emission from transition-metal-dichalcogenide metasurfaces. Nature communications\| PubMed ID: 34552076	2021
Programmable structured surfaces can change the future of wireless communications. Light, science & applications\| PubMed ID: 35764625	2022
Sum-Frequency Generation in High-Q GaP Metasurfaces Driven by Leaky-Wave Guided Modes. Nano letters\| PubMed ID: 35867018	2022
Localized Nanopore Fabrication via Controlled Breakdown. Nanomaterials (Basel, Switzerland)\| PubMed ID: 35889608	2022
Visible-Band Chiroptical Meta-devices with Phase-Change Adjusted Optical Chirality. Nano letters\| PubMed ID: 36112094	2022
Electrically programmable solid-state metasurfaces via flash localised heating. Light, science & applications\| PubMed ID: 36810847	2023
Optical Monitoring of Iron Loading into Single, Native Ferritin Proteins. Nano letters\| PubMed ID: 37053043	2023
Structural Flexibility and Disassembly Kinetics of Single Ferritin Molecules Using Optical Nanotweezers. ACS nano\| PubMed ID: 38850556	2024
Broadband infrared imaging governed by guided-mode resonance in dielectric metasurfaces. Light, science & applications\| PubMed ID: 39256381	2024
Advances in nonlinear metasurfaces for imaging, quantum, and sensing applications. Nanophotonics (Berlin, Germany)\| PubMed ID: 39634716	2023
Quasi-bound states in the continuum with a stable resonance wavelength in dimer dielectric metasurfaces. Nanophotonics (Berlin, Germany)\| PubMed ID: 39635691	2023

Mohsen Rahmani

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