Characterization of commercial thermoelectric modules for precision heat flux measurement.

In this article, we present a cost-effective approach to the precision measurement of heat flux using commercial thermoelectric modules (TEMs). Two different methods of measuring heat flux with TEMs are investigated, namely, passive mode based on the Seebeck effect and active mode based on the Peltier effect. For both modes, a TEM as a heat flux meter is calibrated to show a linear relation between the voltage across the TEM and the heat flux from 0 to ∼450 W m-2. While both modes exhibit sufficiently high sensitivities suitable for low heat flux measurement, active mode is shown to be ∼7 times more sensitive than passive mode. From the speculation on the origin of the measurement uncertainty, we propose a dual TEM scheme by operating the top TEM in passive mode while its bottom temperature maintains constant by the feedback-controlled bottom TEM. The dual TEM scheme can suppress the sensitivity uncertainty up to 3 times when compared to the single-TEM passive mode by stabilizing the bottom temperature. The response time of a 15 × 15 mm2 TEM is measured to be 8.9 ± 1.0 s for heating and 10.8 ± 0.7 s for cooling, which is slower than commercial heat flux meters but still fast enough to measure heat flux with a time resolution on the order of 10 s. We believe that the obtained results can facilitate the use of a commercial TEM for heat flux measurement in various thermal experiments.

Nanostructured chromium-based broadband absorbers and emitters to realize thermally stable solar thermophotovoltaic systems.

The efficiency of traditional solar cells is constrained due to the Shockley-Queisser limit, to circumvent this theoretical limit, the concept of solar thermophotovoltaics (STPVs) has been introduced. The typical design of an STPV system consists of a wideband absorber with its front side facing the sun. The back of this absorber is physically attached to the back of a selective emitter facing a low-bandgap photovoltaic (PV) cell. We demonstrate an STPV system consisting of a wideband absorber and emitter pair achieving a high absorptance of solar radiation within the range of 400-1500 nm (covering the visible and infrared regions), whereas the emitter achieves an emittance of >95% at a wavelength of 2.3 µm. This wavelength corresponds to the bandgap energy of InGaAsSb (0.54 eV), which is the targeted PV cell technology for our STPV system design. The material used for both the absorber and the emitter is chromium due to its high melting temperature of 2200 K. An absorber and emitter pair is also fabricated and the measured results are in agreement with the simulated results. The design achieves an overall solar-to-electrical simulated efficiency of 21% at a moderate temperature of 1573 K with a solar concentration of 3000 suns. Furthermore, an efficiency of 15% can be achieved at a low temperature of 873 K with a solar concentration of 500 suns. The designs are also insensitive to polarization and show negligible degradation in solar absorptance and thermal emittance with a change in the angle of incidence.

Temperature sensitivity of scattering-type near-field nanoscopic imaging in the visible range.

Due to its superb imaging spatial resolution and spectroscopic viability, scattering-type scanning near-field optical microscopy (s-SNOM) has proven to be widely applicable for nanoscale surface imaging and characterization. However, limited works have investigated the sensitivity of the s-SNOM signal to sample temperature. This paper reports the sample temperature effect on the non-interferometric (self-homodyne) s-SNOM scheme at a visible wavelength (λ=638 nm). Our s-SNOM measurements for an arrayed vanadium/quartz sample demonstrate a monotonic decrease in signal intensity as sample temperature increases. As a result, s-SNOM imaging cannot distinguish quartz or vanadium when the sample is heated to ∼309 K: all signals are close to the root-mean-square noise of the detection scheme used for this study (i.e., 19 µV-rms). While further studies are required to better understand the underlying physics of such temperature dependence, the obtained results suggest that s-SNOM measurements should be carefully conducted to meet a constant sample temperature condition, particularly when a visible-spectrum laser is to be used as the light source.

Feedback control of local hotspot temperature using resistive on-substrate nanoheater/thermometer.

This article reports the active control of a local hotspot temperature for accurate nanoscale thermal transport measurement. To this end, we have fabricated resistive on-substrate nanoheater/thermometer (NH/T) devices that have a sensing area of ∼350 nm × 300 nm. Feedback-controlled temporal heating and cooling experiments of the NH/T device confirm that the feedback integral gain plays a dominant role in device's response time for various setpoint temperatures. To further verify the integration of the feedback controller with the NH/T devices, a local tip-induced cooling experiment is performed by scanning a silicon tip over the hotspot area in an atomic force microscope platform. By carefully optimizing the feedback gain and the tip scan speed, we can control the hotspot temperature with the accuracy of ∼±1 K for a broad range of setpoints from 325 K to 355 K. The obtained tip-substrate thermal conductance, including the effects of solid-solid conduction, water meniscus, air conduction, and near-field thermal radiation, is found to be a slightly increasing function of temperature in the range of 127 ± 25 to 179 ± 16 nW/K. Our work demonstrates the reliable controllability of a local hotspot temperature, which will allow the further improvement of various nanoscale thermal metrologies including scanning thermal microscopy and nanoscale thermometry.

Precision Measurement of Phonon-Polaritonic Near-Field Energy Transfer between Macroscale Planar Structures Under Large Thermal Gradients.

Despite its strong potentials in emerging energy applications, near-field thermal radiation between large planar structures has not been fully explored in experiments. Particularly, it is extremely challenging to control a subwavelength gap distance with good parallelism under large thermal gradients. This article reports the precision measurement of near-field radiative energy transfer between two macroscale single-crystalline quartz plates that support surface phonon polaritons. Our measurement scheme allows the precise control of a gap distance down to 200 nm in a highly reproducible manner for a surface area of 5×5 mm^{2}. We have measured near-field thermal radiation as a function of the gap distance for a broad range of thermal gradients up to ∼156 K, observing more than 40 times enhancement of thermal radiation compared to the blackbody limit. By comparing with theoretical prediction based on fluctuational electrodynamics, we demonstrate that such remarkable enhancement is owing to phonon-polaritonic energy transfer across a nanoscale vacuum gap.

Near-Infrared Responsive Gold-Layersome Nanoshells.

Anionic liposomes coated with cationic polyelectrolyte poly-l-lysine (PLL), or layersomes, were used as soft, self-assembled templates for synthesizing gold nanoshells that absorb near-infrared radiation. The gold nanoshells were formed using two techniques: (a) direct reduction of tetrachloroauric acid on the layersomes and (b) the reduction of a tetrachloroauric acid/potassium carbonate "growth" solution on nanosized gold seeds bound to the surface of layersomes. The resulting structures were characterized by transmission and scanning electron microscopy and visible-near-infrared spectroscopy. Direct reduction produced discrete gold nanoparticles on the layersomes. The slower reduction from the growth solution on the gold seeds resulted in more complete shells. The absorption spectra of these suspensions were sensitive to the synthesis method. The morphology of the gold shells was tuned for absorption at biologically safe and tissue-penetrating NIR wavelengths, and laser irradiation at 810 nm produced significant heat. These gold-layersome nanoshells have the potential to be used for photothermal therapy, photothermally mediated drug delivery, and biomedical imaging.

Patchy Layersomes Formed by Layer-by-Layer Coating of Liposomes with Strong Biopolyelectrolytes.

Layer-by-layer deposition of polyelectrolytes (PEs) onto self-assembled liposomes represents an alternative to PE deposition on solid particles for the formation of hollow nanoscale capsules. This work examines how competition between PE-liposome and inter-PE interactions drives the structure and colloidal stability of layersomes. Unlike solid particles, liposomes respond to adsorbed material through lipid reorganization and changes in size and shape. This responsive nature could yield new types of layered PE structures. We show that sequential deposition of strong biopolyelectrolytes, dextran sulfate-sodium salt (DxS-) and poly-l-arginine (PA+), onto cationic liposomes in water yields the expected charge inversion behavior commonly observed for dispersed particles. However, cryogenic transmission electron microscopy results show that the layersomes formed and their PE coatings were heterogeneous. The PE coatings contained PE complexes (PECs) that were formed when an even number of layers (2 or 4) was deposited. PECs remained attached as patches that were spatially distinguishable. This behavior was confirmed through fluorescence anisotropy measurements of liposome bilayer fluidity, where PA+ counteracted the ordering effects of DxS- on the lipid bilayer through charge neutralization and local PEC desorption. With increased charge screening, DxS- desorbed from the layersomes, whereas the patchy layersomes terminating in PA+ retained their PE coatings and colloidal stability at higher salt concentrations. To our knowledge, this is the first time such patchy layersome structures have been observed.

Hollow Microtube Resonators via Silicon Self-Assembly toward Subattogram Mass Sensing Applications.

Fluidic resonators with integrated microchannels (hollow resonators) are attractive for mass, density, and volume measurements of single micro/nanoparticles and cells, yet their widespread use is limited by the complexity of their fabrication. Here we report a simple and cost-effective approach for fabricating hollow microtube resonators. A prestructured silicon wafer is annealed at high temperature under a controlled atmosphere to form self-assembled buried cavities. The interiors of these cavities are oxidized to produce thin oxide tubes, following which the surrounding silicon material is selectively etched away to suspend the oxide tubes. This simple three-step process easily produces hollow microtube resonators. We report another innovation in the capping glass wafer where we integrate fluidic access channels and getter materials along with residual gas suction channels. Combined together, only five photolithographic steps and one bonding step are required to fabricate vacuum-packaged hollow microtube resonators that exhibit quality factors as high as ∼ 13,000. We take one step further to explore additionally attractive features including the ability to tune the device responsivity, changing the resonator material, and scaling down the resonator size. The resonator wall thickness of ∼ 120 nm and the channel hydraulic diameter of ∼ 60 nm are demonstrated solely by conventional microfabrication approaches. The unique characteristics of this new fabrication process facilitate the widespread use of hollow microtube resonators, their translation between diverse research fields, and the production of commercially viable devices.

Laser-assisted photothermal heating of a plasmonic nanoparticle-suspended droplet in a microchannel.

The present article reports the numerical and experimental investigations on the laser-assisted photothermal heating of a nanoliter-sized droplet in a microchannel when plasmonic particles are suspended in the droplet. Plasmonic nanoparticles exhibit strong light absorption and scattering upon the excitation of localized surface plasmons (LSPs), resulting in intense and rapid photothermal heating in a microchannel. Computational models are implemented to theoretically verify the photothermal behavior of gold nanoshell (GNS) and gold nanorod (GNR) particles suspended in a liquid microdroplet. Experiments were conducted to demonstrate rapid heating of a sub-100 nL droplet up to 100 °C with high controllability and repeatability. The heating and cooling time to the steady state is on the order of 1 second, while cooling requires less time than heating. The effects of core parameters, such as nanoparticle structure, volumetric concentration, microchannel depth, and laser power density on heating are studied. The obtained results can be integrated into existing microfluidic technologies that demand accurate and rapid heating of microdroplets in a microchannel.

Temperature measurements of heated microcantilevers using scanning thermoreflectance microscopy.

We report the development of scanning thermoreflectance thermometry and its application for steady and dynamic temperature measurement of a heated microcantilever. The local thermoreflectance signal of the heated microcantilever was calibrated to temperature while the cantilever was under steady and periodic heating operation. The temperature resolution of our approach is 0.6 K, and the spatial resolution is 2 µm, which are comparable to micro-Raman thermometry. However, the temporal resolution of our approach is about 10 µsec, which is significantly faster than micro-Raman thermometry. When the heated microcantilever is periodically heated with frequency up to 100 kHz, we can measure both the in-phase and out-of-phase components of the temperature oscillation. For increasing heating frequency, the measured cantilever AC temperature distribution tends to be confined in the vicinity of the heater region and becomes increasingly out of phase with the driving signal. These results compare well with finite element simulations.

Surface and magnetic polaritons on two-dimensional nanoslab-aligned multilayer structure.

The present study theoretically investigates the radiative properties of a two-dimensional (2-D) multilayer structure that has a dielectric spacer between a metallic substrate and square cross-sectional metallic gratings. Differently from the one-dimensional metallic strips coated on a dielectric spacer atop an opaque metallic film [Opt. Express 16, 11328 (2008)], the 2-D metallic gratings can support the localized surface plasmon in addition to the propagating surface plasmon along the metal-dielectric interface. Moreover, the presence of a dielectric spacer also allows the excitation of magnetic polaritons. Underlying mechanisms of the surface and magnetic polartions on the proposed structure are elucidated by employing the 2-D rigorous coupled-wave analysis. The results obtained in this study will advance our fundamental understanding of light-matter interaction at the nanometer scale and will facilitate the development of engineered nanostructures for real-world applications, such as thermophotovoltaic and photovoltaic devices.

Design analysis of doped-silicon surface plasmon resonance immunosensors in mid-infrared range.

This paper reports the design analysis of a microfabricatable mid-infrared (mid-IR) surface plasmon resonance (SPR) sensor platform. The proposed platform has periodic heavily doped profiles implanted into intrinsic silicon and a thin gold layer deposited on top, making a physically flat grating SPR coupler. A rigorous coupled-wave analysis was conducted to prove the design feasibility, characterize the sensor's performance, and determine geometric parameters of the heavily doped profiles. Finite element analysis (FEA) was also employed to compute the electromagnetic field distributions at the plasmon resonance. Obtained results reveal that the proposed structure can excite the SPR on the normal incidence of mid-IR light, resulting in a large probing depth that will facilitate the study of larger analytes. Furthermore, the whole structure can be microfabricated with well-established batch protocols, providing tunability in the SPR excitation wavelength for specific biosensing needs with a low manufacturing cost. When the SPR sensor is to be used in a Fourier-transform infrared (FTIR) spectroscopy platform, its detection sensitivity and limit of detection are estimated to be 3022 nm/RIU and ~70 pg/mm(2), respectively, at a sample layer thickness of 100 nm. The design analysis performed in the present study will allow the fabrication of a tunable, disposable mid-IR SPR sensor that combines advantages of conventional prism and metallic grating SPR sensors.

Routine femtogram-level chemical analyses using vibrational spectroscopy and self-cleaning scanning probe microscopy tips.

Simultaneous structural and chemical characterization of materials at the nanoscale is both an immediate need and an ongoing challenge. This article reports a route to address this need, which can be rapidly adopted by practitioners, by combining the benefits of widely available scanning probe microscopy and vibrational microspectrometry. In an atomic force microscope (AFM), the probe tip can provide a nanoscale topographic image. Here, we use a temperature-controlled probe tip to selectively acquire an analyte from a specified location and determine its mass in a thermogravimetric manner. The tip is then analyzed via complementary Raman and Fourier transform infrared microspectrometers, providing a molecular characterization of samples down to the femtogram level in minutes. The probe can be self-cleaned and employed for repeated use by rapidly heating it to vaporize the analyte. By combining the established analytical modalities of AFM and vibrational spectrometry, a complete physical and molecular characterization of nanoscale domains is possible: mass determination is facile, thermal analyses can be integrated on the probe, and the obtained spectral data can be related to existing knowledge bases.

Topography imaging with a heated atomic force microscope cantilever in tapping mode.

This article describes tapping mode atomic force microscopy (AFM) using a heated AFM cantilever. The electrical and thermal responses of the cantilever were investigated while the cantilever oscillated in free space or was in intermittent contact with a surface. The cantilever oscillates at its mechanical resonant frequency, 70.36 kHz, which is much faster than its thermal time constant of 300 micros, and so the cantilever operates in thermal steady state. The thermal impedance between the cantilever heater and the sample was measured through the cantilever temperature signal. Topographical imaging was performed on silicon calibration gratings of height 20 and 100 nm. The obtained topography sensitivity is as high as 200 microVnm and the resolution is as good as 0.5 nmHz(1/2), depending on the cantilever power. The cantilever heating power ranges 0-7 mW, which corresponds to a temperature range of 25-700 degrees C. The imaging was performed entirely using the cantilever thermal signal and no laser or other optics was required. As in conventional AFM, the tapping mode operation demonstrated here can suppress imaging artifacts and enable imaging of soft samples.