Ultra-broadband enhancement of nonlinear optical processes from randomly patterned super absorbing metasurfaces.

Broadband light trapping and field localization is highly desired in enhanced light-matter interaction, especially in harmonic generations. However, due to the limited resonant bandwidth, most periodic plasmonic nanostructures cannot cover both fundamental excitation wavelength and harmonic generation wavelength simultaneously. Therefore, most previously reported plasmonic nonlinear optical processes are low in conversion efficiency. Here, we report a strong enhancement of second harmonic generation based on a three-layered super absorbing metasurface structure consisting of a dielectric spacer layer sandwiched by an array of random metallic nanoantennas and a metal ground plate. Intriguingly, the strong light trapping band (e.g. >80%) was realized throughout the entire visible to near-infrared spectral regime (i.e., from 435 nm to 1100 nm), enabling plasmonically enhanced surface harmonic generation and frequency mixing across a broad range of excitation wavelengths, which cannot be achieved with narrow band periodic plasmonic structures. By introducing hybrid random antenna arrays with small metallic nanoparticles and ultra-thin nonlinear optical films (e.g. TiO2) into the nanogaps, the nonlinear optical process can be further enhanced. This broadband light-trapping metastructure shows its potential as a building block for emerging nonlinear optical meta-atoms.

Frozen "Tofu" Effect: Engineered Pores of Hydrophilic Nanoporous Materials.

Frozen tofu is a famous Asian food made by freezing soft bean curds, which are naturally porous to store flavor and nutrients. When the narrow pores of the soft bean curd are saturated with water and then frozen, pore widths expand to generate a completely new porous structure-frozen tofu has visibly wider pores than the initial bean curd. Intriguingly, this principle can be generalized and applied to manipulate micro/nanopores of functional porous materials. In this work, we will manipulate the pore size of nanoporous polymeric photonic crystals based on the phase change between water and ice. Wet-drying and freeze-drying methods were applied to shrink or expand the pore size intentionally. This principle is validated by directly observing the optical reflection peak shift of the material. Owing to the change in pore size, the reflection peak of the polymeric photonic crystal structure can be permanently, and intentionally, tuned. This simple but elegant mechanism is promising for the development of smart materials/devices for applications ranging from oil/water membrane separations, health monitoring, and medical diagnostics to environmental monitoring, anticounterfeiting, and smart windows.

Mn(2+)-Doped CdSe/CdS Core/Multishell Colloidal Quantum Wells Enabling Tunable Carrier-Dopant Exchange Interactions.

In this work, we report the manifestations of carrier-dopant exchange interactions in colloidal Mn(2+)-doped CdSe/CdS core/multishell quantum wells. The carrier-magnetic ion exchange interaction effects are tunable through wave function engineering. In our quantum well heterostructures, manganese was incorporated by growing a Cd0.985Mn0.015S monolayer shell on undoped CdSe nanoplatelets using the colloidal atomic layer deposition technique. Unlike previously synthesized Mn(2+)-doped colloidal nanostructures, the location of the Mn ions was controlled with atomic layer precision in our heterostructures. This is realized by controlling the spatial overlap between the carrier wave functions with the manganese ions by adjusting the location, composition, and number of the CdSe, Cd1-xMnxS, and CdS layers. The photoluminescence quantum yield of our magnetic heterostructures was found to be as high as 20% at room temperature with a narrow photoluminescence bandwidth of ∼22 nm. Our colloidal quantum wells, which exhibit magneto-optical properties analogous to those of epitaxially grown quantum wells, offer new opportunities for solution-processed spin-based semiconductor devices.

Creating diversified response profiles from a single quenchometric sensor element by using phase-resolved luminescence.

We report a new strategy for generating a continuum of response profiles from a single luminescence-based sensor element by using phase-resolved detection. This strategy yields reliable responses that depend in a predictable manner on changes in the luminescent reporter lifetime in the presence of the target analyte, the excitation modulation frequency, and the detector (lock-in amplifier) phase angle. In the traditional steady-state mode, the sensor that we evaluate exhibits a linear, positive going response to changes in the target analyte concentration. Under phase-resolved conditions the analyte-dependent response profiles: (i) can become highly non-linear; (ii) yield negative going responses; (iii) can be biphasic; and (iv) can exhibit super sensitivity (e.g., sensitivities up to 300 fold greater in comparison to steady-state conditions).

Enhanced performance from a hybrid quenchometric deoxyribonucleic acid (DNA) silica xerogel gaseous oxygen sensing platform.

A complex of salmon milt deoxyribonucleic acid (DNA) and the cationic surfactant cetyltrimethylammonium (CTMA) forms an organic-soluble biomaterial that can be readily incorporated within an organically modified silane-based xerogel. The photoluminescence (PL) intensity and excited-state luminescence lifetime of tris(4,7'-diphenyl-1,10'-phenanathroline) ruthenium(II) [(Ru(dpp)3](2+), a common O2 responsive luminophore, increases in the presence of DNA-CTMA within the xerogel. The increase in the [Ru(dpp)3](2+)excited-state lifetime in the presence of DNA-CTMA arises from DNA intercalation that attenuates one or more non-radiative processes, leading to an increase in the [Ru(dpp)3](2+) excited-state lifetime. Prospects for the use of these materials in an oxygen sensor are demonstrated.

Simultaneous multiple wavelength upconversion in a core-shell nanoparticle for enhanced near infrared light harvesting in a dye-sensitized solar cell.

The efficiency of most photovoltaic devices is severely limited by near-infrared (NIR) transmission losses. To alleviate this limitation, a new type of colloidal upconversion nanoparticles (UCNPs), hexagonal core-shell-structured ß-NaYbF4:Er(3+)(2%)/NaYF4:Nd(3+)(30%), is developed and explored in this work as an NIR energy relay material for dye-sensitized solar cells (DSSCs). These UCNPs are able to harvest light energy in multiple NIR regions, and subsequently convert the absorbed energy into visible light where the DSSCs strongly absorb. The NIR-insensitive DSSCs show compelling photocurrent increases through binary upconversion under NIR light illumination either at 785 or 980 nm, substantiating efficient energy relay by these UCNPs. The overall conversion efficiency of the DSSCs was improved with the introduction of UCNPs under simulated AM 1.5 solar irradiation.

Spinning light on the nanoscale.

Light beams with orbital angular momentum have significant potential to transform many areas of modern photonics from imaging to classical and quantum communication systems. We design and experimentally demonstrate an ultracompact array of nanowaveguides with a circular graded distribution of channel diameters that coverts a conventional laser beam into a vortex with an orbital angular momentum. The proposed nanoscale beam converter is likely to enable a new generation of on-chip or all-fiber structured light applications.

Concealing with structured light.

While making objects less visible (or invisible) to a human eye or a radar has captured people's imagination for centuries, current attempts towards realization of this long-awaited functionality range from various stealth technologies to recently proposed cloaking devices. A majority of proposed approaches share a number of common deficiencies such as design complexity, polarization effects, bandwidth, losses and the physical size or shape requirement complicating their implementation especially at optical frequencies. Here we demonstrate an alternative way to conceal macroscopic objects by structuring light itself. In our approach, the incident light is transformed into an optical vortex with a dark core that can be used to conceal macroscopic objects. Once such a beam passed around the object it is transformed back into its initial Gaussian shape with minimum amplitude and phase distortions. Therefore, we propose to use that dark core of the vortex beam to conceal an object that is macroscopic yet small enough to fit the dark (negligibly low intensity) region of the beam. The proposed concealing approach is polarization independent, easy to fabricate, lossless, operates at wavelengths ranging from 560 to 700 nm, and can be used to hide macroscopic objects providing they are smaller than vortex core.

Holographic photopolymer linear variable filter with enhanced blue reflection.

A single beam one-step holographic interferometry method was developed to fabricate porous polymer structures with controllable pore size and location to produce compact graded photonic bandgap structures for linear variable optical filters. This technology is based on holographic polymer dispersed liquid crystal materials. By introducing a forced internal reflection, the optical reflection throughout the visible spectral region, from blue to red, is high and uniform. In addition, the control of the bandwidth of the reflection resonance, related to the light intensity and spatial porosity distributions, was investigated to optimize the optical performance. The development of portable and inexpensive personal health-care and environmental multispectral sensing/imaging devices will be possible using these filters.

Manipulating complex light with metamaterials.

Recent developments in the field of metamaterials have revealed unparalleled opportunities for "engineering" space for light propagation; opening a new paradigm in spin- and quantum-related phenomena in optical physics. Here we show that unique optical properties of metamaterials (MMs) open unlimited prospects to "engineer" light itself. We propose and demonstrate for the first time a novel way of complex light manipulation in few-mode optical fibers using optical MMs. Most importantly, these studies highlight how unique properties of MMs, namely the ability to manipulate both electric and magnetic field components of electromagnetic (EM) waves, open new degrees of freedom in engineering complex polarization states of light at will, while preserving its orbital angular momentum (OAM) state. These results lay the first steps in manipulating complex light in optical fibers, likely providing new opportunities for high capacity communication systems, quantum information, and on-chip signal processing.

Photopatternable transparent conducting oxide nanoparticles for transparent electrodes.

We report a method to fabricate tailored transparent electrodes using photopatternable transparent conducting oxide nanoparticles (TCO NPs). We demonstrate solution-processed micropatterns by a conventional photolithography technique. We have synthesized indium tin oxide (ITO) NPs and functionalized them with a photolabile group, such as t-butoxycarbonyl (t-BOC), which can be deprotected by a chemical amplification reaction in the solid state film. The chemical amplification reaction leads to a shortening of the ligand that changes the solubility of the resulting ITO films. This ligand shortening process also contributes to a reduction of the sheet resistance in the resulting photopatterned ITO films. Furthermore, we have demonstrated the general viability and strength of this approach by also photopatterning zinc oxide (ZnO) NPs.

Filterless optical oxygen sensor based on a CMOS buried double junction photodiode.

We present a custom CMOS IC with a buried double junction (BDJ) photodiode to detect and process the optical signal, eliminating the need for any off-chip optical filters. The on-chip signal processing circuitry improves the desired signal extraction from the optical background noise. Since the IC is manufactured using standard commercial fabrication processes with no post-processing necessary, the system can ultimately be low cost to fabricate. Additionally, because of the CMOS integration, it will consume little power when operating, and even less during stand-by.

One-step fabrication of graded rainbow-colored holographic photopolymer reflection gratings.

A one-step fabrication method has been developed to realize graded holographic photopolymer reflection gratings with gradually varied period in the lateral direction, leading to a rainbow-colored reflection image in the same viewing angle. This low-cost rainbow-colored filter can be integrated with detectors or imaging devices to realize compact and portable spectroscopic analyzers.

Hybrid oxygen-responsive reflective Bragg grating platforms.

Oxygen responsive sensor platforms were fabricated by pin printing tris(4,7-diphenyl-1,10-phenanthroline)ruthenium(II) ([Ru(dpp)(3)](2+)) doped sols onto wavelength tuned reflective Bragg gratings. In an epi-luminescence configuration, these Bragg gratings (Gr) were designed to selectively reflect the O(2) responsive [Ru(dpp)(3)](2+) emission toward the detector to enhance the detected signal magnitude. The xerogel based sensors were formed onto (i) glass (XGl), (ii) directly on top of the grating (XGrGl), or (iii) on the glass substrate opposite the grating (XGlGr). The results show that all sensors exhibit linear, statistically equivalent O(2) sensitivities, and the XGrGl platform yields up to an 8-fold increase in relative detected analytical signal (RDAS) in comparison to the control (XGl) platform.

Optical fiber metamagnetics.

To date, magnetic and negative-index metamaterials at optical frequencies were realized on bulk substrates in the form of thin films with thicknesses on the order of, or less than, optical wavelengths. In this work, we design and experimentally demonstrate, for the first time, fiber-coupled magnetic metamaterials integrated on the transverse cross-section of an optical fiber. Such fiber-metamaterials integration may provide fundamentally new solutions for photonic-on-a-chip systems for sensing, subwavelength imaging, image processing, and biomedical applications.

Image geometric corrections for a new EMCCD-based dual modular x-ray imager.

An EMCCD-based dual modular x-ray imager was recently designed and developed from the component level, providing a high dynamic range of 53 dB and an effective pixel size of 26 µm for angiography and fluoroscopy. The unique 2 × 1 array design efficiently increased the clinical field of view, and also can be readily expanded to an MxN array implementation. Due to the alignment mismatches between the EMCCD sensors and the fiber optic tapers in each module, the output images or video sequences result in a misaligned 2048 × 1024 digital display if uncorrected. In this paper, we present a method for correcting display registration using a custom-designed two layer printed circuit board. This board was designed with grid lines to serve as the calibration pattern, and provides an accurate reference and sufficient contrast to enable proper display registration. Results show an accurate and fine stitching of the two outputs from the two modules.

Optical Demonstration of a Medical Imaging System with an EMCCD-Sensor Array for Use in a High Resolution Dynamic X-ray Imager.

Use of an extensible array of Electron Multiplying CCDs (EMCCDs) in medical x-ray imager applications was demonstrated for the first time. The large variable electronic-gain (up to 2000) and small pixel size of EMCCDs provide effective suppression of readout noise compared to signal, as well as high resolution, enabling the development of an x-ray detector with far superior performance compared to conventional x-ray image intensifiers and flat panel detectors. We are developing arrays of EMCCDs to overcome their limited field of view (FOV). In this work we report on an array of two EMCCD sensors running simultaneously at a high frame rate and optically focused on a mammogram film showing calcified ducts. The work was conducted on an optical table with a pulsed LED bar used to provide a uniform diffuse light onto the film to simulate x-ray projection images. The system can be selected to run at up to 17.5 frames per second or even higher frame rate with binning. Integration time for the sensors can be adjusted from 1 ms to 1000 ms. Twelve-bit correlated double sampling AD converters were used to digitize the images, which were acquired by a National Instruments dual-channel Camera Link PC board in real time. A user-friendly interface was programmed using LabVIEW to save and display 2K × 1K pixel matrix digital images. The demonstration tiles a 2 × 1 array to acquire increased-FOV stationary images taken at different gains and fluoroscopic-like videos recorded by scanning the mammogram simultaneously with both sensors. The results show high resolution and high dynamic range images stitched together with minimal adjustments needed. The EMCCD array design allows for expansion to an M×N array for arbitrarily larger FOV, yet with high resolution and large dynamic range maintained.

Component Level Modular Design of a Solid State X-ray Image Intensifier for an M×N Array.

The Solid-State X-ray Image Intensifier (SSXII) is a novel dynamic x-ray imager, based on an array of electron-multiplying CCDs (EMCCDs), that can significantly improve performance compared to conventional x-ray image intensifiers (XIIs) and flat panel detectors (FPDs). To expand the field-of-view (FOV) of the SSXII detectors while maintaining high resolution, a scalable component level modular design is presented. Each module can be fit together with minimum dead-space and optically coupled to one contiguous x-ray converter plate. The electronics of each of the modules consists of a detachable head-board, on which is mounted the EMCCD, and a driver board. The size of the head-boards is minimized to ensure that the modules fit together properly. The driver boards connect with the head-boards via flat cables and are designed to be plugged into the main mother-board that contains an FPGA chip that generates the driving clock signals for the EMCCDs and analog-to-digital converter (ADC). At the front-end, a high speed ADC on each of the driver boards samples and digitizes the EMCCD analog output signal and an extensible modular digital multiplexer back-end is used to acquire and combine image data from multiple modules. The combined digital data is then transmitted to a PC via a standard Camera Link interface. Eventually, this modular design will be extended to a 3×3 or larger array to accomplish full clinical FOVs and enable the SSXII to replace conventional lower-resolution XIIs or FPDs.

Influence of non-reactive solvent on optical performance, photopolymerization kinetics and morphology of nanoporous polymer gratings.

A study of nanoporous polymer gratings, with controllable nanostructured porosity, as a function of grating performance, photopolymerization kinetics and morphology is presented. Modifying the standard holographic polymer dispersed liquid crystal (H-PDLC) system, by including a non-reactive solvent, results in a layered, nanoporous morphology and produces reflective optical elements with excellent optical performance of broadband reflection. The addition of the non-reactive solvent in the pre-polymer mixture results in a morphology typified by void/polymer layer-by-layer structures if sufficient optical energy is used during the holographic writing process. The duration and intensity of optical exposure necessary to form well-aligned nanoporous structures can only be obtained in the modified system by (a) illumination under longer time of holographic interference patterning (30 min) or (b) illumination under very short time of holographic interference patterning (30 s) and followed by post-curing using homogeneous optical exposure for 60 min. Comparatively, a typical H-PDLC is formed in less than 1 min. To further understand the differences in the formation of these two analogous materials, the temporal dynamics of the photoinitiation and polymerization (propagation) kinetics were examined. It is shown herein that the writing exposure gives a cross-linked polymer network that is denser in the bright regions. With 60% (or even 45%) acrylate conversion, almost no free monomer would be left after the writing. Continued exposure serves primarily to add cross-links. This has the tendency to collapse the network, especially the less dense portions, which in effect get glued down to the more dense parts. To the extent that the solvent increases the mobility of the polymer network, this process will be aided. Equally important, the size of the periodic nanopores can be varied from 10 to 50 nm by controlling either the LC concentration in the pre-polymer mixture or by controlling the time of the homogeneous post-cure.

Quantum Performance Analysis of an EMCCD-based X-ray Detector Using Photon Transfer Technique.

The low electronic noise, high resolution, and good temporal performance of electron-multiplying CCDs (EMCCDs) are ideally suited for applications traditionally served by x-ray image intensifiers. In order to improve an expandable clinical detector's field-of-view and have full control of the system performance, we have successfully built a solid-state x-ray detector. The photon transfer technique was used to quantify the EMCCD quantum performance in terms of sensitivity (or camera gain constant, K), read noise (RN), full-well capacity (FW), and dynamic range (DR). Measured results show the system maintains a K of 11.3 ± 0.9 e(-)/DN at unit gain, with a read noise of 71.5±6.0 e(-)rms at gain 1, which decreases proportionally with higher gains. The full well capacity was measured to be 31.3±2.7 ke(-), providing a dynamic range of 52.8±0.7 dB using the chip manufacturer specified clocking scheme. Similar performance was measured with other commercial camera systems. The manufacturer data sheet indicates a dynamic range of 66 dB is plausible with improved read noise and full well capacity. Different clocking schemes are under investigation to assess their impact on improving performance towards idealized values. EMCCD driver clock voltage levels were adjusted individually to check the influence on quantum performance. The clocks work to transfer charge from the image area to readout amplifier through the storage area, horizontal and multiplication registers. Results indicate that the clock that contributes to lateral overflow drain bias is essential to the system performance in terms of dynamic range and full well capacity. The serial register clocks used for transporting charge stored in the pixels of the memory lines to the output amplifier had the largest effect on RN, while others had less of an impact. Initial adjustment of these clocks resulted in a variability of 16% in the performance of dynamic range, 38% in read noise and 56% in full well capacity. Quantifying the quantum performance provides valuable insight into overall performance and enables optimal adjustment of the clocking scheme. Further improvements are expected.