Surface plasmons are electromagnetic waves that can exist at metal interfaces because of coupling between light and free electrons. Restricted to travel along the interface, these waves can be channeled, concentrated, or otherwise manipulated by surface patterning. However, because surface roughness and other inhomogeneities have so far limited surface-plasmon propagation in real plasmonic devices, simple high-throughput methods are needed to fabricate high-quality patterned metals. We combined template stripping with precisely patterned silicon substrates to obtain ultrasmooth pure metal films with grooves, bumps, pyramids, ridges, and holes. Measured surface-plasmon-propagation lengths on the resulting surfaces approach theoretical values for perfectly flat films. With the use of our method, we demonstrated structures that exhibit Raman scattering enhancements above 10(7) for sensing applications and multilayer films for optical metamaterials.
Metallic nanostructures now play an important role in many applications. In particular, for the emerging fields of plasmonics and nanophotonics, the ability to engineer metals on nanometric scales allows the development of new devices and the study of exciting physics. This review focuses on top-down nanofabrication techniques for engineering metallic nanostructures, along with computational and experimental characterization techniques. A variety of current and emerging applications are also covered.
Colloidal semiconductor nanocrystals have attracted significant interest for applications in solution-processable devices such as light-emitting diodes and solar cells. However, a poor understanding of charge transport in nanocrystal assemblies, specifically the relation between electrical conductance in dark and under light illumination, hinders their technological applicability. Here we simultaneously address the issues of 'dark' transport and photoconductivity in films of PbS nanocrystals, by incorporating them into optical field-effect transistors in which the channel conductance is controlled by both gate voltage and incident radiation. Spectrally resolved photoresponses of these devices reveal a weakly conductive mid-gap band that is responsible for charge transport in dark. The mechanism for conductance, however, changes under illumination when it becomes dominated by band-edge quantized states. In this case, the mid-gap band still has an important role as its occupancy (tuned by the gate voltage) controls the dynamics of band-edge charges.
Multidrug-resistant bacterial infections are an ever-growing threat because of the shrinking arsenal of efficacious antibiotics. Metal nanoparticles can induce cell death, yet the toxicity effect is typically nonspecific. Here, we show that photoexcited quantum dots (QDs) can kill a wide range of multidrug-resistant bacterial clinical isolates, including methicillin-resistant Staphylococcus aureus, carbapenem-resistant Escherichia coli, and extended-spectrum β-lactamase-producing Klebsiella pneumoniae and Salmonella typhimurium. The killing effect is independent of material and controlled by the redox potentials of the photogenerated charge carriers, which selectively alter the cellular redox state. We also show that the QDs can be tailored to kill 92% of bacterial cells in a monoculture, and in a co-culture of E. coli and HEK 293T cells, while leaving the mammalian cells intact, or to increase bacterial proliferation. Photoexcited QDs could be used in the study of the effect of redox states on living systems, and lead to clinical phototherapy for the treatment of infections.
Inexpensive, reproducible and high-throughput fabrication of nanometric apertures in metallic films can benefit many applications in plasmonics, sensing, spectroscopy, lithography and imaging. Here we use template stripping to pattern periodic nanohole arrays in optically thick, smooth Ag films with a silicon template made via nanoimprint lithography. Ag is a low-cost material with good optical properties, but it suffers from poor chemical stability and biocompatibility. However, a thin silica shell encapsulating our template-stripped Ag nanoholes facilitates biosensing applications by protecting the Ag from oxidation as well as providing a robust surface that can be readily modified with a variety of biomolecules using well-established silane chemistry. The thickness of the conformal silica shell can be precisely tuned by atomic layer deposition, and a 15-nm-thick silica shell can effectively prevent fluorophore quenching. The Ag nanohole arrays with silica shells can also be bonded to polydimethylsiloxane (PDMS) microfluidic channels for fluorescence imaging, formation of supported lipid bilayers, and real-time, label-free SPR sensing. Additionally, the smooth surfaces of the template-stripped Ag films enhance refractive index sensitivity compared with as-deposited, rough Ag films. Because nearly centimeter-sized nanohole arrays can be produced inexpensively without using any additional lithography, etching or lift-off, this method can facilitate widespread applications of metallic nanohole arrays for plasmonics and biosensing.
Upconversion of infrared radiation into visible light has been investigated for applications in photovoltaics and biological imaging. However, low conversion efficiency due to small absorption cross-section for infrared light (Yb(3+)), and slow rate of energy transfer (to Er(3+) states) has prevented application of upconversion photoluminescence (UPL) for diffuse sunlight or imaging tissue samples. Here, we utilize resonant surface plasmon polaritons (SPP) waves to enhance UPL in doped-lanthanide nanocrystals. Our analysis indicates that SPP waves not only enhance the electromagnetic field, and hence weak Purcell effect, but also increase the rate of resonant energy transfer from Yb(3+) to Er(3+) ions by 6 fold. While we do observe strong metal mediated quenching (14-fold) of green fluorescence on flat metal surfaces, the nanostructured metal is resonant in the infrared and hence enhances the nanocrystal UPL. This strong Coulombic effect on energy transfer can have important implications for other fluorescent and excitonic systems too.
We demonstrate three-dimensional plasmonic nanofocusing of light with patterned metallic pyramids obtained via template stripping. Gratings on the faces of these pyramids convert linearly polarized light into plasmons that propagate toward and converge at a approximately 10 nm apex. Experiments and computer simulations confirm that optical energy is focused into a nanoscale volume (5 x 10(-5) wavelength(3)). Because these structures are easily and reproducibly fabricated, our results could benefit many applications, including imaging, sensing, lithography, and nonlinear spectroscopy.
A simple route to flat, large-area, single-crystalline films for plasmonics is demonstrated by sputter deposition of silver onto mica substrates at elevated temperatures. The films exhibit improved dielectric properties and allow more precise patterning of high-quality nanostructures for plasmonic applications.
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