Capillary Transfer of Self-Assembled Colloidal Crystals.

Colloidal self-assembly has attracted significant interest in numerous applications including optics, electrochemistry, thermofluidics, and biomolecule templating. To meet the requirements of these applications, numerous fabrication methods have been developed. However, these are limited to narrow ranges of feature sizes, are incompatible with many substrates, and/or have low scalability, significantly limiting the use of colloidal self-assembly. In this work, we study the capillary transfer of colloidal crystals and demonstrate that this approach overcomes these limitations. Enabled by capillary transfer, we fabricate 2D colloidal crystals with nano-to-micro feature sizes spanning 2 orders of magnitude and on typically challenging substrates including those that are hydrophobic, rough, curved, or structured with microchannels. We developed and systemically validated a capillary peeling model, elucidating the underlying transfer physics. Due to its high versatility, good quality, and simplicity, this approach can expand the possibilities of colloidal self-assembly and enhance the performance of applications using colloidal crystals.

Tailoring the Desorption Behavior of Hygroscopic Gels for Atmospheric Water Harvesting in Arid Climates.

The ubiquitous nature of atmospheric moisture makes it a significant water resource available at any geographical location. Atmospheric water harvesting (AWH) technology, which extracts moisture from the ambient air to generate clean water, is a promising strategy to realize decentralized water production. The high water uptake by salt-based sorbents makes them attractive for AWH, especially in arid environments. However, they often have relatively high desorption heat, rendering water release an energy-intensive process. A  LiCl-incorporating polyacrylamide hydrogel (PAM-LiCl) capable of effective moisture harvesting from arid environments is proposed. The interactions between the hydrophilic hydrogel network and the captured water generate more free and weakly bonded water, significantly lowering the desorption heat compared with conventional neat salt sorbents. Benefiting from the affinity for swelling of the polymer backbones, the developed PAM-LiCl achieves a high water uptake of ≈1.1 g g-1 at 20% RH with fast sorption kinetics of ≈0.008 g g-1  min-1  and further demonstrates a daily water yield up to ≈7 g g-1 at this condition. These findings provide a new pathway for the synthesis of materials with efficient water absorption/desorption properties, to reach energy-efficient water release for AWH in arid climates.

High contrast cleavage detection.

Photonic biosensors that use optical resonances to amplify signals from refractive index changes offer high sensitivity, real-time readout, and scalable, low-cost fabrication. However, when used with classic affinity assays, they struggle with noise from nonspecific binding and are limited by the low refractive index and small size of target biological molecules. In this Letter, we evaluate the performance of an integrated microring photonic biosensor using the high contrast cleavage detection (HCCD) mechanism, which we recently introduced. The HCCD sensors make use of dramatic optical signal amplification caused by the cleavage of large numbers of high-contrast nanoparticle reporters instead of the adsorption of labeled or unlabeled low-index biological molecules. We evaluate the advantages of the HCCD detection mechanism over conventional target-capture detection techniques with the same label and the same sensor platform, using an example of a silicon ring resonator as an optical transducer decorated with silicon nanoparticles as high-contrast reporters. In the practical realization of this detection scheme, detection specificity and signal amplification can be achieved via collateral nucleic acid cleavage caused by enzymes such as CRISPR Cas12a and Cas13 after binding to a target DNA/RNA sequence in solution.

Inverse design of a single-frequency diffractive biosensor based on the reporter cleavage detection mechanism.

Vertically interrogated porous silicon (PSi) interferometric biosensors have shown high potential for sensing bio-molecules as they combine high detection sensitivity with simplicity of fabrication, functionalization, optical coupling, and interfacing with microfluidic systems. However, most interferometric sensor designs require either broadband or wavelength-tunable light sources as well as wide-angle detection schemes, increasing their complexity and cost for point-of-care biosensing applications. The limit of detection of such sensors is also constrained by the small size and low refractive index of biological molecules, making it hard to detect very low concentrations of pathogens. In this work, we use a large-scale computational "inverse design" technique to demonstrate a single-frequency, fixed-angle PSi-based biosensor, which exploits a recently developed high-contrast reporter cleavage detection (HCCD) technique. The HCCD sensors detect high-index reporter cleavage events instead of low-index target analyte capture events as typical for traditional label-free optical biosensors. We use the inverse design approach to discover an optimal configuration of a PSi biosensor that makes use of the extended achievable range of cleavage-induced PSi effective index variations and can be interrogated at a single frequency and at a fixed angle. The optimized design in the form of a one-dimensional PSi grating exhibits the change in the reflectance up to 55 % at the interrogation angle of 12∘ and wavelength of 600 nm, which is caused by cleavage of Au nanoparticle reporters initially occupying 2% of the sensor surface area. The maximum possible change in reflectance is predicted to be 222 % (for a two-dimensional freeform design not amenable to fabrication). This demonstration may pave the way for developing new or redesigned conventional interferometric and colorimetric point-of-care biosensor systems in combination with the cleavage-based detection schemes.

High contrast cleavage detection for enhancing porous silicon sensor sensitivity.

Using porous silicon (PSi) interferometer sensors, we show the first experimental implementation of the high contrast cleavage detection (HCCD) mechanism. HCCD makes use of dramatic optical signal amplification caused by cleavage of high-contrast nanoparticle labeled reporters instead of the capture of low-index biological molecules. An approximately 2 nm reflectance peak shift was detected after cleavage of DNA-quantum dot reporters from the PSi surface via exposure to a 12.5 nM DNase enzyme solution. This signal change is 20 times greater than the resolution of the spectrometer used for the interferometric measurements, and the interferometric measurements agree with the response predicted by simulations and fluorescence measurements. These proof of principle experiments show a clear path to achieving a real-time, highly sensitive readout for a broad range of biological diagnostic assays that generate a signal via nucleic acid cleavage triggered by specific molecular binding events.

Self-powered broadband photo-detection and persistent energy generation with junction-free strained Bi2Te3 thin films.

We experimentally demonstrate efficient broadband self-powered photo-detection and power generation in thin films of polycrystalline bismuth telluride (Bi2Te3) semiconductors under inhomogeneous strain. The developed simple, junction-free, lightweight, and flexible photo-detectors are composed of a thin active layer and Ohmic contacts on a flexible plastic substrate, and can operate at room temperature and without application of an external bias voltage. We attribute the observed phenomena to the generation of an electric field due to a spontaneous polarization produced by strain gradient, which can separate both photo-generated and thermally-generated charge carriers in bulk of the semiconductor material, without a semiconductor junction. We show that the developed photo-detectors can generate electric power during both the daytime and the nighttime, by either harnessing solar and thermal radiation or by emitting thermal radiation into the cold sky. To the best of our knowledge, this is the first demonstration of the power generation in a simple junction-free device under negative illumination, which exhibits higher voltage than the previously used expensive commercial HgCdTe photo-diode. Significant improvements in the photo-detector performance are expected if the low-charge-mobility polycrystalline active layer is replaced with high-quality single-crystal material. The technology is not limited to Bi2Te3 as the active material, and offers many potential applications in night vision, wearable sensors, long-range LIDAR, and daytime/nighttime energy generation technologies.

Spectral, spatial and polarization-selective perfect absorbers with large magnetic response for sensing and thermal emission control.

Spectral, spatial, and polarization selective perfect absorption of light in periodic metal-dielectric-metal nanoslits, each of which supporting a single electric-field anti-symmetric surface mode, is systematically studied. Our numerical analysis shows complete absorption of p-polarized light associated with large magnetic field enhancement at wavelengths from the visible to the mid-infrared range and roles played by the geometrical parameters of the structure. This understanding is then applied to the design of the structure with multiple nanoslits in a period that exhibits complete absorption at multiple wavelengths. Semi-analytical expression of the zeroth mode reflectance is derived, which shows a good agreement with numerical simulations and yields clear insight into the underlying physics of light-matter interactions in the structure.

Contactless steam generation and superheating under one sun illumination.

Steam generation using solar energy provides the basis for many sustainable desalination, sanitization, and process heating technologies. Recently, interest has arisen for low-cost floating structures that absorb solar radiation and transfer energy to water via thermal conduction, driving evaporation. However, contact between water and the structure leads to fouling and pins the vapour temperature near the boiling point. Here we demonstrate solar-driven evaporation using a structure not in contact with water. The structure absorbs solar radiation and re-radiates infrared photons, which are directly absorbed by the water within a sub-100 µm penetration depth. Due to the physical separation from the water, fouling is entirely avoided. Due to the thermal separation, the structure is no longer pinned at the boiling point, and is used to superheat the generated steam. We generate steam with temperatures up to 133 °C, demonstrating superheated steam in a non-pressurized system under one sun illumination.

Sensitive singular-phase optical detection without phase measurements with Tamm plasmons.

Spectrally-tailored interactions of light with material interfaces offer many exciting applications in sensing, photo-detection, and optical energy conversion. In particular, complete suppression of light reflectance at select frequencies accompanied by sharp phase variations in the reflected signal forms the basis for the development of ultra-sensitive singular-phase optical detection schemes such as Brewster and surface plasmon interferometry. However, both the Brewster effect and surface-plasmon-mediated absorption on planar interfaces are limited to one polarization of the incident light and oblique excitation angles, and may have limited bandwidth dictated by the material dielectric index and plasma frequency. To alleviate these limitations, we design narrow-band super-absorbers composed of plasmonic materials embedded into dielectric photonic nanostructures with topologically-protected interfacial Tamm plasmon states. These structures have planar geometry and do not require nanopatterning to achieve perfect absorption of both polarizations of the incident light in a wide range of incident angles, including the normal incidence. Their absorption lines are tunable across a very broad spectral range via engineering of the photon bandstructure of the dielectric photonic nanostructures to achieve reversal of the geometrical phase across the interface with the plasmonic absorber. We outline the design strategy to achieve perfect absorptance in Tamm structures with dissipative losses via conjugate impedance matching. We further demonstrate via modeling how these structures can be engineered to support sharp asymmetric amplitude resonances, which can be used to improve the sensitivity of optical sensors in the amplitude-only detection scheme that does not require use of bulky and expensive ellipsometry equipment.

Toward a High-Efficient Utilization of Solar Radiation by Quad-Band Solar Spectral Splitting.

The promising quad-band solar spectral splitter incorporates the properties of the optical filter and the spectrally selective solar thermal absorber can direct PV band to PV modules and absorb thermal band energy for thermal process with low thermal losses. It provides a new strategy for spectral splitting and offers potential ways for hybrid PVT system design.

Entropic and Near-Field Improvements of Thermoradiative Cells.

A p-n junction maintained at above ambient temperature can work as a heat engine, converting some of the supplied heat into electricity and rejecting entropy by interband emission. Such thermoradiative cells have potential to harvest low-grade heat into electricity. By analyzing the entropy content of different spectral components of thermal radiation, we identify an approach to increase the efficiency of thermoradiative cells via spectrally selecting long-wavelength photons for radiative exchange. Furthermore, we predict that the near-field photon extraction by coupling photons generated from interband electronic transition to phonon polariton modes on the surface of a heat sink can increase the conversion efficiency as well as the power generation density, providing more opportunities to efficiently utilize terrestrial emission for clean energy. An ideal InSb thermoradiative cell can achieve a maximum efficiency and power density up to 20.4% and 327 Wm-2, respectively, between a hot source at 500 K and a cold sink at 300 K. However, sub-bandgap and non-radiative losses will significantly degrade the cell performance.

Control of radiative processes for energy conversion and harvesting.

We review recent advances in the fundamental understanding and technological applications of radiative processes for energy harvesting, conversion, efficiency, and sustainability. State-of-the-art and remaining challenges are discussed, together with the latest developments outlined in the papers comprising this focus issue. The topics range from the fundamentals of the thermal emission manipulation in the far and near field, to applications in radiative cooling, thermophotovoltaics, thermal rectification, and novel approaches to photon detection and conversion.

Directed Assembly of Optoplasmonic Hybrid Materials with Tunable Photonic-Plasmonic Properties.

Optoplasmonic materials are metallo-dielectric hybrid structures that combine metallic and dielectric components in defined geometries in which plasmonic and photonic modes synergistically interact. These beneficial interactions can be harnessed by integrating plasmonic nanoantennas into defined photonic environments generated, for instance, by discrete optical resonators or extended systems of diffractively coupled nanoparticles. Optoplasmonic structures facilitate photonic-plasmonic mode coupling and offer degrees of freedom for creating optical fields with predefined amplitude and phase in space and time that are absent in conventional photonic or plasmonic structures. This Perspective reviews the fundamental electromagnetic mechanisms underlying selected optoplasmonic approaches with an emphasis on materials available through template-guided self-assembly strategies.

Thin-film 'Thermal Well' Emitters and Absorbers for High-Efficiency Thermophotovoltaics.

A new approach is introduced to significantly improve the performance of thermophotovoltaic (TPV) systems using low-dimensional thermal emitters and photovoltaic (PV) cells. By reducing the thickness of both the emitter and the PV cell, strong spectral selectivity in thermal emission and absorption can be achieved by confining photons in trapped waveguide modes inside the thin-films that act as thermal analogs to quantum wells. Simultaneously, photo-excited carriers travel shorter distances across the thin-films reducing bulk recombination losses resulting in a lower saturation current in the PV cell. We predict a TPV efficiency enhancement with near-field coupling between the thermal emitter and the PV cell up to 38.7% using a thin-film germanium (Ge) emitter at 1000 K and an ultra-thin gallium antimonide (GaSb) cell supported by perfect back reflectors separated by 100 nm. Even in the far-field limit, the efficiency is predicted to reach 31.5%, which is over an order of magnitude higher than the Shockley Queisser limit of 1.6% for a bulk GaSb cell and a blackbody emitter at 1000 K. The proposed design approach does not require nanoscale patterning of the emitter and PV cell surfaces, but instead offers a simple low-cost solution to improve the performance of thermophotovoltaic systems.

15.7% Efficient 10-µm-thick crystalline silicon solar cells using periodic nanostructures.

Only ten micrometer thick crystalline silicon solar cells deliver a short-circuit current of 34.5 mA cm(-2) and power conversion efficiency of 15.7%. The record performance for a crystalline silicon solar cell of such thinness is enabled by an advanced light-trapping design incorporating a 2D inverted pyramid photonic crystal and a rear dielectric/reflector stack.

Demonstration of efficient on-chip photon transfer in self-assembled optoplasmonic networks.

Plasmonic nanoantennas facilitate the manipulation of light fields on deeply sub-diffraction-limited length scales, but high dissipative losses in metals make new approaches for an efficient energy transfer in extended on-chip integrated plasmonic circuits mandatory. We demonstrate in this article efficient photon transfer in discrete optoplasmonic molecules comprising gold nanoparticle (NP) dimer antennas located in the evanescent field of a 2 µm diameter polystyrene bead, which served as an optical microcavity (OM). The optoplasmonic molecules were generated through a guided self-assembly strategy in which the OMs were immobilized in binding sites generated by quartz (SiO2) or silicon posts that contained plasmonic nanoantennas on their tips. Control of the post height facilitated an accurate positioning of the plasmonic antennas into the evanescent field of the whispering gallery modes located in the equatorial plane of the OM. Cy3 and Cy5.5 dyes were tethered to the plasmonic antennas through oligonucleotide spacers to act as on-chip light sources. The intensity of Cy3 was found to be increased relative to that of Cy5.5 in the vicinity of the plasmonic antennas where strongly enhanced electric field intensity and optical density of states selectively increase the excitation and emission rates of Cy3 due to spectral overlap with the plasmon. The fluorescent dyes preferentially emitted into the OM, which efficiently trapped and recirculated the photons. We experimentally determined a relative photon transfer efficiency of 44% in non-optimized self-assembled optoplasmonic molecules in this proof-of-principle study.

Enhanced light focusing in self-assembled optoplasmonic clusters with subwavelength dimensions.

Compact metallo-dielectric hybrid clusters with subwavelength dimensions are fabricated by template guided self-assembly. Elastic and inelastic scattering spectroscopy and electromagnetic simulations reveal that hybrid clusters comprising TiO(2) nanoparticles on top of a cluster of strongly coupled gold nanoparticles harness synergistic electromagnetic interactions between the building blocks. This results in a boost of the peak electric field intensity and a redistribution of the field in the ambient medium. The complex phase landscape in the clusters features optical vortices that enhance the magnetic field.

Ultrasensitive detection of a protein by optical trapping in a photonic-plasmonic microcavity.

Microcavity and whispering gallery mode (WGM) biosensors derive their sensitivity from monitoring frequency shifts induced by protein binding at sites of highly confined field intensities, where field strengths can be further amplified by excitation of plasmon resonances in nanoparticle layers. Here, we propose a mechanism based on optical trapping of a protein at the site of plasmonic field enhancements for achieving ultra sensitive detection in only microliter-scale sample volumes, and in real-time. We demonstrate femto-Molar sensitivity corresponding to a few 1000 s of macromolecules. Simulations based on Mie theory agree well with the optical trapping concept at plasmonic 'hotspots' locations.

Quantification of differential ErbB1 and ErbB2 cell surface expression and spatial nanoclustering through plasmon coupling.

Cell surface receptors play ubiquitous roles in cell signaling and communication and their expression levels are important biomarkers for many diseases. Expression levels are, however, only one factor that determines the physiological activity of a receptor. For some surface receptors, their distribution on the cell surface, especially their clustering, provides additional mechanisms for regulation. To access this spatial information robust assays are required that provide detailed insight into the organization of cell surface receptors on nanometer length scales. In this manuscript, we demonstrate through combination of scattering spectroscopy, electron microscopy, and generalized multiple particle Mie theory (GMT) simulations that the density- and morphology-dependent spectral response of Au nanoparticle (NP) immunolabels bound to the epidermal growth factor receptors ErbB1 and ErbB2 encodes quantitative information of both the cell surface expression and spatial clustering of the two receptors in different unliganded in vitro cancer cell lines (SKBR3, MCF7, A431). A systematic characterization of the collective spectral responses of NPs targeted at ErbB1 and ErbB2 at various NP concentrations indicates differences in the large-scale organization of ErbB1 and ErbB2 in cell lines that overexpress these receptors. Validation experiments in the scanning electron microscope (SEM) confirm that NPs targeted at ErbB1 on A431 are more strongly clustered than NPs bound to ErbB2 on SKBR3 or MCF7 at overall comparable NP surface densities. This finding is consistent with the existence of larger receptor clusters for ErbB1 than for ErbB2 in the plasma membranes of the respective cells.