skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Hybrid interfacial cryosoret nano-engineering in photonic resonator interferometric scattering microscopy: Insights from nanoparticles and nano-assemblies
The requirements of augmented signal contrast provided by nanoparticle tags in biosensor microscopy-based point-of-care technologies for cancer and infectious disease diagnostics can be addressed through metallo-dielectric nanoarchitectures that enhance optical scattering and absorption to provide digital resolution detection of single tags with simple instrumentation. Photonic Resonator Interferometric Scattering Microscopy (PRISM) enables label-free visualization of nanometer-scale analytes such as extracellular vesicles and virions, and its applicability can be extended to biomolecular analyte counting through nanoparticle tags. Here, we present template-free, linker-less cryosoret nano-assemblies fabricated via adiabatic cooling (−196 °C) as plasmonic nano-antennas that provide high scattering contrast in PRISM. Plasmonic Ag and Au nanomaterials and their cryosorets are evaluated through imaging experiments and simulations based on the finite element method to understand the photo-plasmonic coupling effect at the surface of a photonic crystal (PC) interface. The Ag and Au cryosorets provide at most 8.29-fold and 6.77-fold higher signal contrast compared to their singlet counterpart. Through the simulations, the averaged field magnitude enhancements of 2.77-fold and 3.68-fold are observed for Ag and Au cryosorets when interfacing with PCs compared to bare glass substrates. The hybrid coupling between the localized Mie and delocalized Bragg plasmons of cryosorets and the underlying PC's guided mode resonance provides insights for developing nano-assembly-based nano-tags for biosensing applications.  more » « less
Award ID(s):
1900277 2232681
PAR ID:
10532056
Author(s) / Creator(s):
; ;
Publisher / Repository:
AIP Publishing
Date Published:
Journal Name:
Applied Physics Letters
Volume:
124
Issue:
23
ISSN:
0003-6951
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Interferometric scattering microscopy is increasingly employed in biomedical research owing to its extraordinary capability of detecting nano-objects individually through their intrinsic elastic scattering. To significantly improve the signal-to-noise ratio without increasing illumination intensity, we developed photonic resonator interferometric scattering microscopy (PRISM) in which a dielectric photonic crystal (PC) resonator is utilized as the sample substrate. The scattered light is amplified by the PC through resonant near-field enhancement, which then interferes with the <1% transmitted light to create a large intensity contrast. Importantly, the scattered photons assume the wavevectors delineated by PC’s photonic band structure, resulting in the ability to utilize a non-immersion objective without significant loss at illumination density as low as 25 W cm−2. An analytical model of the scattering process is discussed, followed by demonstration of virus and protein detection. The results showcase the promise of nanophotonic surfaces in the development of resonance-enhanced interferometric microscopies. 
    more » « less
  2. Plasmonic and photonic technologies have attracted strong interest in the past few decades toward several interdisciplinary applications stemming from unique light-matter interactions fostered by materials at the nanoscale. The versatility of plasmonic and photonic sensors for ultrasensitive, rapid, analyte sensing without extensive sample pre-treatment steps or sophisticated optics have resulted in their strong foothold in the broad arena of biosensing. Fluorescence-based bioanalytical techniques are widely used in liquid-biopsy diagnostics applications, but require many labeled target molecules to combine their emission output to achieve a practically useful signal-to-noise ratio. Approaches capable of amplifying fluorescence signals can provide signal-to-noise sufficient for digitally counting single emitters for ultrasensitive assays that are detected with simple and inexpensive instruments. [1]. Plasmonic and nano-photonics can function in synergy to amplify fluorescence signals. By concentrating optical energy well below the diffraction limit, plasmonic nanoantenna provide spatial control over excitation light, but their quality factor (Q) is modulated by radiative and dissipative losses. Photonic crystals (PC) as dielectric microcavities have a diffraction-limited optical mode volume despite being able to generate a high Q-factor. Here, we demonstrate a plasmonic-photonic hybrid system to produce a much stronger fluorescent enhancement for digital resolution biosensing. With an optimized dielectric spacer layer, around 200 Alexa-647 fluorophores have been coated over heterometallic Ag@Au core-shell plasmonic nanostructures with minimized Ohmic losses and quenching effects [2]. The target-specific molecule capture events enabled this plasmonic fluor to attach to the PC surface, forming a Plasmonic-Photonic hybrid mode. With much stronger local field enhancement, far-field directional emission, large Purcell enhancement, and high quantum efficiency, we report a two-orders signal enhancement from PC-enhanced plasmonic-fluor (104-fold brighter than a single fluorophore). This improved signal-to-noise ratio enabled us to perform single molecule imaging even with a 10x (NA=0.2) objective lens while offering 3 orders of magnitude boost in the limit of detection of Interleukine-6 (common biomarker for cancer, inflammation, sepsis, and autoimmune disease) compared with standard immunoassays in human plasma 
    more » « less
  3. Abstract Quantum state control of two‐level emitters is fundamental for many information processing, metrology, and sensing applications. However, quantum‐coherent photonic control of solid‐state emitters has traditionally been limited to cryogenic environments, which are not compatible with implementation in scalable, broadly distributed technologies. In contrast, plasmonic nano‐cavities with deep sub‐wavelength mode volumes have recently emerged as a path toward room temperature quantum control. However, optimization, control, and modeling of the cavity mode volume are still in their infancy. Here recent demonstrations of plasmonic tip‐enhanced strong coupling (TESC) with a configurable nano‐tip cavity are extended to perform a systematic experimental investigation of the cavity‐emitter interaction strength and its dependence on tip position, augmented by modeling based on both classical electrodynamics and a quasinormal mode framework. Based on this work, a perspective for nano‐cavity optics is provided as a promising tool for room temperature control of quantum coherent interactions that could spark new innovations in fields from quantum information and quantum sensing to quantum chemistry and molecular opto‐mechanics. 
    more » « less
  4. Abstract Silver nanowires (AgNWs) hold great promise for applications in wearable electronics, flexible solar cells, chemical and biological sensors, photonic/plasmonic circuits, and scanning probe microscopy (SPM) due to their unique plasmonic, mechanical, and electronic properties. However, the lifetime, reliability, and operating conditions of AgNW-based devices are significantly restricted by their poor chemical stability, limiting their commercial potentials. Therefore, it is crucial to create a reliable oxidation barrier on AgNWs that provides long-term chemical stability to various optical, electrical, and mechanical devices while maintaining their high performance. Here we report a room-temperature solution-phase approach to grow an ultra-thin, epitaxial gold coating on AgNWs to effectively shield the Ag surface from environmental oxidation. The Ag@Au core-shell nanowires (Ag@Au NWs) remain stable in air for over six months, under elevated temperature and humidity (80 °C and 100% humidity) for twelve weeks, in physiological buffer solutions for three weeks, and can survive overnight treatment of an oxidative solution (2% H 2 O 2 ). The Ag@Au core-shell NWs demonstrated comparable performance as pristine AgNWs in various electronic, optical, and mechanical devices, such as transparent mesh electrodes, surface-enhanced Raman spectroscopy (SERS) substrates, plasmonic waveguides, plasmonic nanofocusing probes, and high-aspect-ratio, high-resolution atomic force microscopy (AFM) probes. These Au@Ag core-shell NWs offer a universal solution towards chemically-stable AgNW-based devices without compromising material property or device performance. 
    more » « less
  5. The complex nature and structure of biomolecules and nanoparticles and their interactions make it challenging to achieve a deeper understanding of the dynamics at the nano–bio interface of enzymes and plasmonic nanoparticles subjected to light excitation. In this study, circular dichroism (CD) and Raman spectroscopic experiments and molecular dynamics (MD) simulations were used to investigate the potential changes at the nano–bio interface upon plasmonic excitation. Our data showed that photothermal and thermal heating induced distinct changes in the secondary structure of a model nanobioconjugate composed of lipase fromCandida antarcticafraction B (CALB) and gold nanoparticles (AuNPs). The use of a green laser led to a substantial decrease in the α-helix content of the lipase from 66% to 13% and an increase in the β-sheet content from 5% to 31% compared to the initial conformation of the nanobioconjugate. In contrast, the differences under similar thermal heating conditions were only 55% and 11%, respectively. This study revealed important differences related to the enzyme secondary structure, enzyme–nanoparticle interactions, and the stability of the enzyme catalytic triad (Ser105-Asp187-His224), influenced by the instantaneous local temperature increase generated from photothermal heating compared to the slower rate of thermal heating of the bulk. These results provide valuable insights into the interactions between biomolecules and plasmonic nanoparticles induced by photothermal heating, advancing plasmonic biocatalysis and related fields. 
    more » « less