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TiO2 Nano-Biopatterning Reveals Optimal Ligand Presentation for Cell-Matrix Adhesion Formation

Jain, Kashish; Pandey, Ashish; Wang, Hao; Chung, Taerin; Nemati, Arash; Kanchanawong, Pakorn; Sheetz, Michael P; Cai, Haogang; Changede, Rishita
Nanoscale organization of transmembrane receptors is becoming recognized as critical for cellular functions, enabled by the nanoscale engineering of bioligand presentation. Previously, a spatial threshold of ≤60 nm for integrin binding ligands in cell-matrix adhesion was demonstrated using mono-ligand gold nanoparticles. However, the ligand geometric arrangement was limited to hexagonal arrays of mono-ligands, while plasmonic quenching by gold limited further investigation by fluorescence-based high-resolution imaging. Here, these limitations were overcome with dielectric TiO2 nanopatterns, which allows fine-tuning ligand cluster size, eliminating fluorescence quenching, thus enabling super-resolution fluorescence microscopy on nanopatterns. By dual-color super-resolution imaging, high precision and consistency among nanopatterns, bioligands, and integrin nanoclusters was observed validating the high quality and integrity of both nanopattern functionalization and passivation. By screening TiO2 nanodiscs with various diameters, an increase in fibroblast cell adhesion, spreading area, and YAP nuclear localization on 100nm-diameter compared with smaller diameters was observed, and Focal Adhesion Kinase was identified as the regulatory signal. These findings explore the optimal ligand presentation when the minimal requirements are sufficiently fulfilled in the heterogenous ECM network of isolated binding regions with abundant ligands. Integration of high-fidelity nano-biopatterning with super-resolution imaging will allow precise quantitative studies to address early signaling events in response to receptor clustering and their nanoscale organization. This article is protected by copyright. All rights reserved.
PMID: 38340044
ISSN: 1521-4095
CID: 5632172

Dielectric metasurfaces for next-generation optical biosensing: a comparison with plasmonic sensing

Chung, Taerin; Wang, Hao; Cai, Haogang
In the past decades, nanophotonic biosensors have been extended from the extensively studied plasmonic platforms to dielectric metasurfaces. Instead of plasmonic resonance, dielectric metasurfaces are based on Mie resonance, and provide comparable sensitivity with superior resonance bandwidth, Q factor, and figure-of-merit. Although the plasmonic photothermal effect is beneficial in many biomedical applications, it is a fundamental limitation for biosensing. Dielectric metasurfaces solve the ohmic loss and heating problems, providing better repeatability, stability, and biocompatibility. We review the high-Q resonances based on various physical phenomena tailored by meta-atom geometric designs, and compare dielectric and plasmonic metasurfaces in refractometric, surface-enhanced, and chiral sensing for various biomedical and diagnostic applications. Departing from conventional spectral shift measurement using spectrometers, imaging-based and spectrometer-less biosensing are highlighted, including single-wavelength refractometric barcoding, surface-enhanced molecular fingerprinting, and integrated visual reporting. These unique modalities enabled by dielectric metasurfaces point to two important research directions. On the one hand, hyperspectral imaging provides massive information for smart data processing, which not only achieve better biomolecular sensing performance than conventional ensemble averaging, but also enable real-time monitoring of cellular or microbial behaviour in physiological conditions. On the other hand, a single metasurface can integrate both functions of sensing and optical output engineering, using single-wavelength or broadband light sources, which provides simple, fast, compact, and cost-effective solutions. Finally, we provide perspectives in future development on metasurface nanofabrication, functionalization, material, configuration, and integration, towards next-generation optical biosensing for ultra-sensitive, portable/wearable, lab-on-a-chip, point-of-care, multiplexed, and scalable applications.
PMID: 37352839
ISSN: 1361-6528
CID: 5535142

A universal metasurface transfer technique for heterogeneous integration

Zhang, Xu; Cai, Haogang; Rezaei, Soroosh Daqiqeh; Rosenmann, Daniel; Lopez, Daniel
Metasurfaces offer a versatile platform for engineering the wavefront of light using nanostructures with subwavelength dimensions and hold great promise for dramatically miniaturizing conventional optical elements due to their small footprint and broad functionality. However, metasurfaces so far have been mainly demonstrated on bulky and planar substrates that are often orders of magnitude thicker than the metasurface itself. Conventional substrates not only nullify the reduced footprint advantage of metasurfaces, but also limit their application scenarios. The bulk substrate also determines the metasurface dielectric environment, with potentially undesired optical effects that undermine the optical performance. Here we develop a universal polymer-assisted transfer technique to tackle this challenge by decoupling the substrate employed on the fabrication of metasurfaces from that used for the target application. As an example, Huygens' metasurfaces with 120 nm thickness in the visible range (532 nm) are demonstrated to be transferred onto a 100 nm thick freestanding SiNx membrane while maintaining excellent structural integrity and optical performance of diffraction-limited focusing. This transfer method not only enables the thinnest dielectric metalens to the best of our knowledge, but also opens up new opportunities in integrating cascaded and multilayer metasurfaces, as well as the heterogeneous integration with nonconventional substrates and various electronic/photonic devices.
PMID: 37383029
ISSN: 2192-8606
CID: 5540422

Gold Nanoparticle Enabled Localized Surface Plasmon Resonance on Unique Gold Nanomushroom Structures for On-Chip CRISPR-Cas13a Sensing

Waitkus, Jacob; Chang, Yu; Liu, Li; Puttaswamy, Srinivasu Valagerahally; Chung, Taerin; Vargas, Adrian M Molina; Dollery, Stephen J; O'Connell, Mitchell R; Cai, Haogang; Tobin, Gregory J; Bhalla, Nikhil; Du, Ke
A novel localized surface plasmon resonance (LSPR) system based on the coupling of gold nanomushrooms (AuNMs) and gold nanoparticles (AuNPs) is developed to enable a significant plasmonic resonant shift. The AuNP size, surface chemistry, and concentration are characterized to maximize the LSPR effect. A 31 nm redshift is achieved when the AuNMs are saturated by the AuNPs. This giant redshift also increases the full width of the spectrum and is explained by the 3D finite-difference time-domain (FDTD) calculation. In addition, this LSPR substrate is packaged in a microfluidic cell and integrated with a CRISPR-Cas13a RNA detection assay for the detection of the SARS-CoV-2 RNA targets. Once activated by the target, the AuNPs are cleaved from linker probes and randomly deposited on the AuNM substrate, demonstrating a large redshift. The novel LSPR chip using AuNP as an indicator is simple, specific, isothermal, and label-free; and thus, provides a new opportunity to achieve the next generation multiplexing and sensitive molecular diagnostic system.
PMID: 37091050
ISSN: 2196-7350
CID: 5464942

Ligand functionalization of titanium nanopattern enables the analysis of cell-ligand interactions by super-resolution microscopy

Jain, Kashish; Kanchanawong, Pakorn; Sheetz, Michael P; Zhou, Xianjing; Cai, Haogang; Changede, Rishita
The spatiotemporal aspects of early signaling events during interactions between cells and their environment dictate multiple downstream outcomes. While advances in nanopatterning techniques have allowed the isolation of these signaling events, a major limitation of conventional nanopatterning methods is its dependence on gold (Au) or related materials that plasmonically quench fluorescence and, thus, are incompatible with super-resolution fluorescence microscopy. Here we describe a novel method that integrates nanopatterning with single-molecule resolution fluorescence imaging, thus enabling mechanistic dissection of molecular-scale signaling events in conjunction with nanoscale geometry manipulation. Our method exploits nanofabricated titanium (Ti) whose oxide (TiO2) is a dielectric material with no plasmonic effects. We describe the surface chemistry for decorating specific ligands such as cyclo-RGD (arginine, glycine and aspartate: a ligand for fibronectin-binding integrins) on TiO2 nanoline and nanodot substrates, and demonstrate the ability to perform dual-color super-resolution imaging on these patterns. Ti nanofabrication is similar to other metallic materials like Au, while the functionalization of TiO2 is relatively fast, safe, economical, easy to set up with commonly available reagents, and robust against environmental parameters such as humidity. Fabrication of nanopatterns takes ~2-3 d, preparation for functionalization ~1.5-2 d, and functionalization 3 h, after which cell culture and imaging experiments can be performed. We suggest that this method may facilitate the interrogation of nanoscale geometry and force at single-molecule resolution, and should find ready applications in early detection and interpretation of physiochemical signaling events at the cell membrane in the fields of cell biology, immunology, regenerative medicine, and related fields.
PMID: 35896742
ISSN: 1750-2799
CID: 5276702

On-Demand Fully Enclosed Superhydrophobic-Optofluidic Devices Enabled by Microstereolithography

Chang, Yu; Bao, Mengdi; Waitkus, Jacob; Cai, Haogang; Du, Ke
Superhydrophobic surface-based optofluidics have been introduced to biosensors and unconventional optics with unique advantages, such as low light loss and power consumption. However, most of these platforms were made with planar-like microstructures and nanostructures, which may cause bonding issues and result in significant waveguide loss. Here, we introduce a fully enclosed superhydrophobic-based optofluidics system, enabled by a one-step microstereolithography procedure. Various microstructured cladding designs with a feature size down to 100 μm were studied and a "T-type" overhang design exhibits the lowest optical loss, regardless of the excitation wavelength. Surprisingly, the optical loss of superhydrophobic-based optofluidics is not solely decided by the solid area fraction at the solid/water/air interface, but also the cross-section shape and the effective cladding layer composition. We show that this fully enclosed optofluidic system can be used for CRISPR-labeled quantum dot quantification, intended for in vitro and in vivo CRISPR therapeutics.
PMID: 35984448
ISSN: 1520-5827
CID: 5300302

Broadband Liquid Crystal Tunable Metasurfaces in the Visible: Liquid Crystal Inhomogeneities across the Metasurface Parameter Space

Dolan, James A.; Cai, Haogang; Delalande, Lily; Li, Xiao; Martinson, Alex B.F.; De Pablo, Juan J.; López, Daniel; Nealey, Paul F.
Optical metasurfaces - planar nanostructured devices that can arbitrarily tailor the wavefront of light - may be reconfigured by changing their dielectric environment. The application of external stimuli to liquid crystals is a particularly promising means of tuning the optical properties of embedded metasurfaces because of liquid crystals' large and broadband optical anisotropy. However, the detailed behavior of liquid crystals immediately adjacent to the nanostructured meta-atoms elements is often overlooked, despite the optics of the device depending sensitively on this behavior (e.g., the spectral position of the meta-atom resonances). This is of increasing concern as the wavelength of operation further approaches the short-wavelength end of the visible spectrum and, therefore, the length scale of the inhomogeneities in the liquid crystal director field. In this manuscript, we undertake a fully comprehensive study, across the metasurface geometrical parameter space, of broadband (450-700 nm) all-dielectric liquid crystal tunable metasurfaces operating in the visible. Through combined experimental characterization, liquid crystal modeling, and optical simulations, we reveal and quantify the improved accuracy with which the optical properties of the liquid crystal tunable metasurfaces may be described, and identify the underlying physical mechanism: the three-dimensional spatial overlap of the liquid crystal director field and metasurface optical near fields in the vicinity of the meta-atoms.
ISSN: 2330-4022
CID: 4796082

Contribution of Ferromagnetic Medium to the Output of Triboelectric Nanogenerators Derived from Maxwell's Equations

Li, Yahui; Li, Guizhong; Zhang, Penglei; Zhang, Haodong; Ren, Chao; Shi, Xian; Cai, Han; Zhang, Yanxin; Wang, Yusen; Guo, Zhanfeng; Li, Hongfang; Ding, Guifu; Cai, Haogang; Yang, Zhuoqing; Zhang, Chi; Wang, Zhong Lin
Triboelectric nanogenerators (TENGs) use the displacement current as a driving force to convert mechanical energy into electric power, which has made great contributions to micro-nano energy harvesting, self-powered systems, and the sustainable development of mankind. To date, it is accepted that the output of TENGs is only dependent on the polarization effect. This study reveals that this view is incomplete and, in reality, the magnetization effect also makes a significant contribution to the output of TENGs. For the first time, a novel insight on the output of TENGs is discovered through the theoretical derivation and analysis of Maxwell's equations in ferromagnetic medium. Experimentally, TENGs based on ferromagnetic media are constructed, which exhibit higher output than that of non-ferromagnetic media based. Interestingly, the output behavior of ferromagnetic media based TENGs is strongly related to the external magnetic field ambient, which is well demonstrated. The discovered output characteristics of TENGs are precisely derived from the working principle of TENGs, simultaneously, a completed and unified theoretical system is constructed for TENGs. This significant discovery and theory will be an indispensable supplement to the existing research on TENGs and also provide a general guidance and deeper understanding of the TENG.
ISSN: 1614-6832
CID: 4859982

Polarization-Insensitive Medium-Switchable Holographic Metasurfaces

Cai, Haogang; Dolan, James A.; Gordon, George S.D.; Chung, Taerin; López, Daniel
The adoption of metasurfaces has led to revolutionary advances in holography due to improved compactness, integrability, and performance. Switchable meta-holograms projecting different replay field images in a controllable manner are highly desirable. Still, existing technologies generally rely on the use of polarized light and additional optics to facilitate switching. Consequently, the potential benefits afforded through the use of metasurfaces are limited both by the system complexity and a fixed relationship between the optical input and output. In this manuscript, we demonstrate polarization-insensitive metasurfaces encoding arbitrary and independent holograms, which can be switched between by changing the refractive index of the infiltration medium while maintaining identical illumination conditions. By sidestepping the requirements for high-performance light sources, switching optics, or delicate alignment, this approach points toward ultracompact and cost-effective switchable meta-holograms for various practical applications, such as holographic image projection, eye-perceptible sensors, optical information storage, processing, and security.
ISSN: 2330-4022
CID: 5008152

Kirigami Engineering-Nanoscale Structures Exhibiting a Range of Controllable 3D Configurations

Zhang, Xu; Medina, Lior; Cai, Haogang; Aksyuk, Vladimir; Espinosa, Horacio D; Lopez, Daniel
Kirigami structures provide a promising approach to transform flat films into 3D complex structures that are difficult to achieve by conventional fabrication approaches. By designing the cutting geometry, it is shown that distinct buckling-induced out-of-plane configurations can be obtained, separated by a sharp transition characterized by a critical geometric dimension of the structures. In situ electron microscopy experiments reveal the effect of the ratio between the in-plane cut size and film thickness on out-of-plane configurations. Moreover, geometrically nonlinear finite element analyses (FEA) accurately predict the out-of-plane modes measured experimentally, their transition as a function of cut geometry, and provide the stress-strain response of the kirigami structures. The combined computational-experimental approach and results reported here represent a step forward in the characterization of thin films experiencing buckling-induced out-of-plane shape transformations and provide a path to control 3D configurations of micro- and nanoscale buckling-induced kirigami structures. The out-of-plane configurations promise great utility in the creation of micro- and nanoscale systems that can harness such structural behavior, such as optical scanning micromirrors, novel actuators, and nanorobotics. This work is of particular significance as the kirigami dimensions approach the sub-micrometer scale which is challenging to achieve with conventional micro-electromechanical system technologies.
PMID: 33349995
ISSN: 1521-4095
CID: 4735282