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WIREs Nanomed Nanobiotechnol
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SERS Nanosensors and Nanoreporters: Golden Opportunities in Biomedical Applications

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This article provides an overview of recent developments and applications of surface‐enhanced Raman scattering (SERS) nanosensors and nanoreporters in our laboratory for use in biochemical monitoring, medical diagnostics, and therapy. The design and fabrication of different types of plasmonics‐active nanostructures are discussed. The SERS nanosensors can be used in various applications including pH sensing, protein detection, and gene diagnostics. For DNA detection the ‘Molecular Sentinel’ nanoprobe can be used as a homogenous bioassay in solution or on a chip platform. Gold nanostars provide an excellent multi‐modality theranostic platform, combining Raman and SERS with two‐photon luminescence (TPL) imaging as well as photodynamic therapy (PDT), and photothermal therapy (PTT). Plasmonics‐enhanced and optically modulated delivery of nanostars into brain tumor in live animals was demonstrated; photothermal treatment of tumor vasculature may induce inflammasome activation, thus increasing the permeability of the blood brain‐tumor barrier. The imaging method using TPL of gold nanostars provides an unprecedented spatial selectivity for enhanced targeted nanostar delivery to cortical tumor tissue. A quintuple‐modality nanoreporter based on gold nanostars for SERS, TPL, magnetic resonance imaging (MRI), computed tomography (CT), and PTT has recently been developed. The possibility of combining spectral selectivity and high sensitivity of the SERS process with the inherent molecular specificity of bioreceptor‐based nanoprobes provides a unique multiplex and selective diagnostic modality. Several examples of optical detection using SERS in combination with other detection and treatment modalities are discussed to illustrate the usefulness and potential of SERS nanosensors and nanoreporters for medical applications. WIREs Nanomed Nanobiotechnol 2015, 7:17–33. doi: 10.1002/wnan.1283 This article is categorized under: Diagnostic Tools > Biosensing Diagnostic Tools > Diagnostic Nanodevices Diagnostic Tools > In Vivo Nanodiagnostics and Imaging
Surface‐enhanced Raman scattering (SERS)‐active plasmonic platforms. (a) Nanowave platform consisting of nanosphere arrays coated with metal film. The inset represents the unit cell used as a 3‐D model for Finite Element Model (FEM) calculations. (b) Metal film on nanorod arrays fabricated using nanolithography and plasma etching. (c) Scanning electron microscopy (SEM) micrograph showing an array of gold nanopillars formed by focused ion beam (FIB) fabrication. Scale bar is 1 µm. (d) White‐light microscopy image of a SERS‐active nanoprobe measuring the intracellular and extracellular pH of a single live MCF‐7 human breast cancer cell. The inset is an SEM image of the Ag Island Film (AgIF)‐coated nanofiber tip. The scale bar is 500 nm long.
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Surface‐enhanced Raman scattering (SERS) spectra of DTTC loaded in silica‐coated gold nanostars injected intradermally and measured in vivo in a rat model.
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(a) Surface‐enhanced Raman scattering (SERS) intensity at 1066 cm−1 of various concentrations of nanoprobes in solution; (b) SERS spectrum from tumor phantom with nanoprobe.
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(a) TAT‐NS cellular uptake in BT 549 cells at 37°C with two different inhibitors (CytoD: cytochalasin D, MβCD: methyl‐β‐cyclodextrin). Active‐dividing cells were incubated 30 min under 37°C in media containing no or two different inhibitors followed by replacing the media (same inhibitor plus TAT‐NS 0.1 nM) for another hour. Cells were fixed by paraformaldehyde and stained with 4′,6‐diamidino‐2‐phenylindole (DAPI) before imaging. Image size 500 µm. (b) Two‐photon luminescence (TPL) imaging of cerebral microangiogram through a cranial window, Hoescht 33342‐stained whole brain, and DAPI (nucleus, blue)/CD31 (endothelium, red)‐stained histology. Mice implanted with brain tumor xenograft were injected with polyethylene glycol (PEG)‐NS (1 ∼ 5 pmole). The microangiogram was performed through a cranial window within 1 h after injection showing high‐resolution vascular patterns. The excised brain and tumor histology were performed 3 days after injection showing accumulation of PEG‐NS within tumor. PEG‐NS extravasated particularly around tumor vessels and at the tumor periphery. Nanostars are white. T, tumor. N, normal. Scale bar: 200 µm.
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(a) Surface‐enhanced Raman scattering (SERRS) spectra from nanostars coated with different NIR dyes (IR780, IR792, IR797, IR813; Sigma‐Aldrich). The spectra were collected using a hand‐held Raman spectrometer (Xantus)‐1, Bayspec with NIR laser (785 nm, 100 mW) and 100 ms integration time. (b) Quantitative multiplexing of four SERRS probes under different mixing ratios in solution. The spectral decomposition was performed by analyzing the whole spectra (wavenumber: 200 ∼ 1500 cm−1) against four reference spectra. A free‐fitting polynomial was introduced to reduce the fitting error. The calculated fractions of each SERRS probe were adjusted to 100% and plotted against the mixing ratio. The spectra were collected using a hand‐held Raman spectrometer (Xantus‐1) with a NIR laser (785 nm, 200 mW) and 500 ms integration time (10 accumulations).
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Demonstration of surface‐enhanced Raman scattering (SERS) signal enhancement from silver‐coated gold nanostar ([email protected]) platform compared to AuNS.
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(A) The operating principle of the plasmonic coupling interference (PCI) approach for nucleic acid detection. (B) Detection of miR‐21 micro RNA (miRNA) molecules using PCI nanoprobes. Curve (a): blank sample containing a mixture of Capture‐NPs and Reporter‐NPs. Curve (b): in the presence of 100 nM non‐complementary DNA as the negative control. Curve (c): in the presence of 100 nM synthetic miR‐21 targets.
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Scheme for two‐multiplex detection of complementary target ssDNA sequences based on molecular sentinel‐on‐chip (MSC) technique.
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(a) Molecular model of para‐mercaptobenzoic acid (pMBA) chosen in the simulation study; (b) Surface‐enhanced Raman scattering (SERS) spectra of pH nanoprobe under pH 5 (black) and pH 9 (red). Arrow markers show spectral positions of SERS peak intensity changes with pH from 5 to 9.
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(a) Field in the gap between two spheres (broken curve) and two spheroids of aspect ratio 2:4. In all three cases, the gap is 10%. The spheroids are equal in volume to that of the sphere; (b) field in the gap between two spheres (broken curve) and two spheroids of aspect ratio 2:4. The gap is 5% of the diameter of the sphere; (c) field in the gap between two spheres (broken curve) and two spheroids of aspect ratio 2:4. The gap is 2% of the diameter of the sphere.
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Diagnostic Tools > Diagnostic Nanodevices
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