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At least 91 records · Page 5

Near Infrared Emitting Semiconductor Polymer Dots for Bioimaging and Sensing

Semiconducting polymer dots (Pdots) are rapidly becoming one of the most studied nanoparticles in fluorescence bioimaging and sensing. Their small size, high brightness, and resistance to photobleaching make them one of the most attractive fluorophores for fluorescence imaging and sensing applications. This paper highlights our recent advances in fluorescence bioimaging and sensing with nanoscale luminescent Pdots, specifically the use of organic dyes as dopant molecules to modify the optical properties of Pdots to enable deep red and near infrared fluorescence bioimaging applications and to impart sensitivity of dye doped Pdots towards selected analytes. Building on our earlier work, we report the formation of secondary antibody-conjugated Pdots and provide Cryo-TEM evidence for their formation. We demonstrate the selective targeting of the antibody-conjugated Pdots to FLAG-tagged FLS2 membrane receptors in genetically engineered plant leaf cells. We also report the formation of a new class of luminescent Pdots with emission wavelengths of around 1000 nm. Finally, we demonstrate the formation and utility of oxygen sensing Pdots in aqueous media.

47 OTHER INSTRUMENTATION↗

Recent development of thermoelectric nanofibers and their composites

This review deals with the recent development of thermoelectric (TE) nanofibers and their composite materials. Typical processing and manufacturing technologies for preparing nanofibers are introduced. Specifically, electrospinning, electrochemical oxidation, and liquid phase chemical deposition approaches are discussed. Various kinds of TE nanofibers are introduced one-by-one. Several important inorganic and organic nanofibers including carbon-based nanofibers, conducting polymer-based nanofibers, and transition metal oxide-based nanofibers with significant thermoelectric responses are shown. Thermoelectric properties of some important nanofibers are compared. The applications of TE nanofibers for energy conversion, thermal imaging and temperature sensing are illustrated. Perspectives and concluding remarks are presented.

42 ENGINEERING↗

A review of quantum imaging methods and enabling technologies

The field of quantum imaging has recently seen an explosion of new methods and techniques. At the heart of most quantum imaging approaches are three enabling technologies: the source of the quantum light, the detectors that turn sensing into imaging, and the method by which the quantum nature of light is leveraged to improve the desired measurement. This review addresses the dominant and emerging technologies in each of these components as well as details concerning the implementations of various quantum imaging methods.

36 MATERIALS SCIENCE↗

Snapshot multispectral imaging using a diffractive optical network

Abstract Multispectral imaging has been used for numerous applications in e.g., environmental monitoring, aerospace, defense, and biomedicine. Here, we present a diffractive optical network-based multispectral imaging system trained using deep learning to create a virtual spectral filter array at the output image field-of-view. This diffractive multispectral imager performs spatially-coherent imaging over a large spectrum, and at the same time, routes a pre-determined set of spectral channels onto an array of pixels at the output plane, converting a monochrome focal-plane array or image sensor into a multispectral imaging device without any spectral filters or image recovery algorithms. Furthermore, the spectral responsivity of this diffractive multispectral imager is not sensitive to input polarization states. Through numerical simulations, we present different diffractive network designs that achieve snapshot multispectral imaging with 4, 9 and 16 unique spectral bands within the visible spectrum, based on passive spatially-structured diffractive surfaces, with a compact design that axially spans ~72 λ m , where λ m is the mean wavelength of the spectral band of interest. Moreover, we experimentally demonstrate a diffractive multispectral imager based on a 3D-printed diffractive network that creates at its output image plane a spatially repeating virtual spectral filter array with 2 × 2 = 4 unique bands at terahertz spectrum. Due to their compact form factor and computation-free, power-efficient and polarization-insensitive forward operation, diffractive multispectral imagers can be transformative for various imaging and sensing applications and be used at different parts of the electromagnetic spectrum where high-density and wide-area multispectral pixel arrays are not widely available.

36 MATERIALS SCIENCE↗

Mechanically flexible mid-wave infrared imagers using black phosphorus ink films

The mid-wave infrared (MWIR) spectral range (λ = 3–8 μm) enables important sensing and imaging applications, including non-invasive bioimaging, night vision, and autonomous navigation. Commercial MWIR photodetectors are limited to rigid imagers based on heteroepitaxial materials. There is an emerging need for mechanically flexible MWIR imagers to broaden their functionality and practicality. Recently, photodetectors using van der Waals (vdW) black phosphorus (BP) flakes have demonstrated highly sensitive room-temperature photodetection. Additionally, vdW materials are solution-processable, facilitating scalable processing and flexible device fabrication. In this work, we present flexible MWIR imagers consisting of photodiodes fabricated on thin plastic substrates using BP ink films. We demonstrate mechanically robust responsivity up to 2.5-mm bending radii and after 5000 bending cycles. Leveraging this flexibility, we achieve full-azimuthal imaging, detecting directional light sources with precision. These results establish a scalable approach for large-area, conformable MWIR imaging and pave the way for integration with flexible electronics.

Wijaya, Theodorus Jonathan↗

Computer vision-based rock bolt detection in orthomosaic imagery obtained in the Waste Isolation Pilot Plant underground facility

Assessing structural integrity of large underground tunnel facilities is often a time consuming and human-labor intensive task. Thus, research using various modes of sensing and automated detection of key structural components in mines is posed to aid in safety assessments and establishing overall structural health. We propose an approach utilizing off-the-shelf camera and lidar technology fixed to a custom sensing platform, image stitching techniques, fine-tuned object detection models, and specialized model-inference methods to automatically detect, count, and map roof bolts for assessment of structural safety in man-made underground tunnels. Results show a novel workflow for effective object counting in orthomosaic tunnel ceiling images generated from collections in GPS-denied mining environments. Additionally, we demonstrate effective fine-tuning of EfficientDet object detectors utilizing state-of-the-art image augmentation techniques known as the mosaic and mixup transformations. Our work is demonstrated on sensed data and imagery collected from the Department of Energy (DOE) Waste Isolation Pilot Plant (WIPP) where miles of tunnel ceiling must be assessed for structural integrity.

42 ENGINEERING↗

Far-field speckle correlations as a function of object position for microscopically distinguishing objects hidden in a randomly scattering medium

Super-resolution optical sensing is of critical importance in science and technology and has required prior information about an imaging system or obtrusive near-field probing. Additionally, coherent imaging and sensing in heavily scattering media such as biological tissue has been challenging, and practical approaches have either been restricted to measuring the field transmission of a single point source, or to where the medium is thin. We present the concept of far-subwavelength spatial sensing with relative object motion in speckle as a means to coherently sense through heavy scatter. Experimental results demonstrate the ability to distinguish nominally identical objects with nanometer-scale translation while hidden in randomly scattering media, without the need for precise or known location and with imprecise replacement. The theory and supportive illustrations presented provide the basis for super-resolution sensing and the possibility of virtually unlimited spatial resolution, including through thick, heavily scattering media with relative motion of an object in a structured field. This work provides enabling opportunities for material inspection, security, and biological sensing.

Hastings, Ryan L. (ORCID:0009000095977807)↗

Monitoring Preferential Flow of Water in Sand Using Thermoacoustics Wave Imaging

Abstract Accurate predictions of fluid flow, mass transport, and reaction rates critically impact the efficiency and reliability of subsurface exploration and sustainable use of subsurface resources. Quantitative dynamical sensing and imaging can play a pivotal role in the ability to make such predictions. Geophysical thermoacoustic technology has the potential to provide the aforementioned capabilities, since it builds upon the principle that electromagnetic and mechanical wave fields can be coupled through a thermodynamic process. In this letter, we present laboratory experiments featuring the efficacy of thermoacoustic imaging in the monitoring of preferential flow of water in porous media. Our laboratory experimental equipment can be readily packaged in a form factor that fits in a borehole, and the use of multiple acoustic transducers—which can be combined with volumetric coding techniques—has the potential to provide quasi‐real‐time imaging (0.5 Hz video rate) of regions in close proximity (a few meters) of an open field well.

Geology↗

Computational Imaging for Intelligence in Highly Scattering Aerosols (Final Report)

Natural and man-made degraded visual environments pose major threats to national security. The random scattering and absorption of light by tiny particles suspended in the air reduces situational awareness and causes unacceptable down-time for critical systems and operations. To improve the situation, we have developed several approaches to interpret the information contained within scattered light to enhance sensing and imaging in scattering media. These approaches were tested at the Sandia National Laboratory Fog Chamber facility and with tabletop fog chambers. Computationally efficient light transport models were developed and leveraged for computational sensing. The models are based on a weak angular dependence approximation to the Boltzmann or radiative transfer equation that appears to be applicable in both the moderate and highly scattering regimes. After the new model was experimentally validated, statistical approaches for detection, localization, and imaging of objects hidden in fog were developed and demonstrated. A binary hypothesis test and the Neyman-Pearson lemma provided the highest theoretically possible probability of detection for a specified false alarm rate and signal-to-noise ratio. Maximum likelihood estimation allowed estimation of the fog optical properties as well as the position, size, and reflection coefficient of an object in fog. A computational dehazing approach was implemented to reduce the effects of scatter on images, making object features more readily discernible. We have developed, characterized, and deployed a new Tabletop Fog Chamber capable of repeatably generating multiple unique fog-analogues for optical testing in degraded visual environments. We characterized this chamber using both optical and microphysical techniques. In doing so we have explored the ability of droplet nucleation theory to describe the aerosols generated within the chamber, as well as Mie scattering theory to describe the attenuation of light by said aerosols, and correlated the aerosol microphysics to optical properties such as transmission and meteorological optical range (MOR). This chamber has proved highly valuable and has supported multiple efforts inclusive to and exclusive of this LDRD project to test optics in degraded visual environments. Circularly polarized light has been found to maintain its polarization state better than linearly polarized light when propagating through fog. This was demonstrated experimentally in both the visible and short-wave infrared (SWIR) by imaging targets made of different commercially available retroreflective films. It was found that active circularly polarized imaging can increase contrast and range compared to linearly polarized imaging. We have completed an initial investigation of the capability for machine learning methods to reduce the effects of light scattering when imaging through fog. Previously acquired experimental long-wave images were used to train an autoencoder denoising architecture. Overfitting was found to be a problem because of lack of variability in the object type in this data set. The lessons learned were used to collect a well labeled dataset with much more variability using the Tabletop Fog Chamber that will be available for future studies. We have developed several new sensing methods using speckle intensity correlations. First, the ability to image moving objects in fog was shown, establishing that our unique speckle imaging method can be implemented in dynamic scattering media. Second, the speckle decorrelation over time was found to be sensitive to fog composition, implying extensions to fog characterization. Third, the ability to distinguish macroscopically identical objects on a far-subwavelength scale was demonstrated, suggesting numerous applications ranging from nanoscale defect detection to security. Fourth, we have shown the capability to simultaneously image and localize hidden objects, allowing the speckle imaging method to be effective without prior object positional information. Finally, an interferometric effect was presented that illustrates a new approach for analyzing speckle intensity correlations that may lead to more effective ways to localize and image moving objects. All of these results represent significant developments that challenge the limits of the application of speckle imaging and open important application spaces. A theory was developed and simulations were performed to assess the potential transverse resolution benefit of relative motion in structured illumination for radar systems. Results for a simplified radar system model indicate that significant resolution benefits are possible using data from scanning a structured beam over the target, with the use of appropriate signal processing.

58 GEOSCIENCES↗

Ultrasensitive Photothermal Spectroscopy: Harnessing the Seebeck Effect for Attogram-Level Detection

Molecular-level spectroscopy is crucial for sensing and imaging applications, yet detecting and quantifying minuscule quantities of chemicals remain a challenge, especially when they surface adsorb in low numbers. Here, we introduce a photothermal spectroscopic technique that enables the high selectivity sensing of adsorbates with an attogram detection limit. Our approach utilizes the Seebeck effect in a microfabricated nanoscale thermocouple junction, incorporated into the apex of a microcantilever. We observe minimal thermal mass exhibited by the sensor, which maintains exceptional thermal insulation. The temperature variation driving the thermoelectric junction arises from the nonradiative decay of molecular adsorbates’ vibrational states on the tip. We demonstrate the detection of photothermal spectra of physisorbed trinitrotoluene (TNT) and dimethyl methylphosphonate (DMMP) molecules, as well as representative polymers, with an estimated mass of 10 -18 g.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Metaoptics Enabled Multifunctional Imaging

Despite the fact that most microorganisms occupy two- and three-dimensional space in heterogeneous arrangements and in proximity to other microorganisms of different species, much of our current knowledge about their metabolic processes is derived from homogenizing, then analyzing, the chemical content of cultures containing a single microbial species. This project addressed this fundamental dichotomy by developing a set of optical imaging principles combining multiple new technologies. The imaging strategies developed in this project combine metaoptics structures with active in situ nanoscale control of the chemical environment and applied them to a microbial system, Myxococcus xanthus, with particular relevance to the DoE mission. The combination of metaoptical architectures and nanoscale control over the molecular environment enables: (a) precise control over the electromagnetic (EM) field at length scales smaller than the wavelength of light; (b) control of the interaction of the EM field with critical molecular systems in DOE relevant microbes; (c) control over the chemical environment – especially the presence and quantity of reactive oxygen species (ROS) that can affect redox homeostasis; and (d) the ability to ask new kinds of questions not accessible to ‘omics’ approaches or standard methods of biological imaging. These capabilities are applicable to detailed studies of metabolic pathways in microbes and to lignocellulosic biomass deconstruction. To accomplish these objectives, we pursued two over-arching technical goals: (1) the development of new metaoptics-enabled approaches to imaging and spectroscopic characterization; and (2) the development of tools to control the chemical environment of a microbial sample with nanometer-scale precision. Goal 1 was addressed through the design, fabrication, and characterization of new metasurfaces capable of super-resolution imaging through extreme confinement of the optical field. Goal 2 was addressed by controlling the redox potential on the nanoscale in microbial communities and characterizing their effect on intrinsic bacterial fluorophores which act as molecular sentinels and through characterization of soluble factors secreted by Myxococcus xanthus by confocal Raman imaging. The optical imaging/sensing approaches developed here make it possible to use these powerful new imaging and sensing modalities in metabolic studies by making it possible to visualize and track the spatial and temporal expression patterns of natural or engineered pathways in microorganisms.

09 BIOMASS FUELS↗

Cognition at the Point of Sensing

Over the last 15 years, compressive sensing techniques have been developed which have the potential to greatly reduce the amount of data collected by systems while preserving the amount of information obtained. A cost of this efficiency is that a computationally-intensive optimization routine must be used to put the sensed data into a form that a person can interpret. At the same time, machine learning techniques have experienced tremendous growth as well. Machines have demonstrated the ability learn how to effectively perform tasks such as detection and classification at speeds much faster than humanly possible. Our goal in this project was to study the feasibility of using compressive sensing systems "at the edge." That is, how can compressive sensing sensors be deployed such that information is created at the remote sensor rather than sending raw data to a central processing location? Studies were performed to analyze whether machine learning could be done on the compressively sensed data in its raw form. If a machine is performing the task, is it possible to do so without putting the data into a human interpretable form? We show that this is possible for some systems, in particular a compressive sensing snapshot imaging spectrometer. Machine learning tasks were demonstrated to be more effective and more robust to noise when the machine learning algorithm worked on data in its raw form. This system is shown to outperform a traditional spectrometer. Techniques for reducing the complexity of the reconstruction routine were also analyzed. Techniques for such as data regularization, deep neural networks, and matrix completion were studied and shown to have benefits over traditional reconstruction techniques. In this project we showed that compressive sensing sensors are indeed feasible at the edge. As always, sensors and algorithms must be carefully tuned to work in the constrained environment. In this project we developed tools and techniques to enable those analyses.

47 OTHER INSTRUMENTATION↗

Unprecedented Fluorophore Photostability Enabled by Low‐Loss Organic Hyperbolic Materials

Abstract The dynamics of photons in fluorescent molecules plays a key role in fluorescence imaging, optical sensing, organic photovoltaics, and displays. Photobleaching is an irreversible photodegradation process of fluorophores, representing a fundamental limitation in relevant optical applications. Chemical reagents are used to suppress the photobleaching rate but with exceptionally high specificity for each type of fluorophore. Here, using organic hyperbolic materials (OHMs), an optical platform to achieve unprecedented fluorophore photostability without any chemical specificity is demonstrated. A more than 500‐fold lengthening of the photobleaching lifetime and a 230‐fold increase in the total emitted photon counts are observed simultaneously. These exceptional improvements solely come from the low‐loss hyperbolic dispersion of OHM films and the large resultant Purcell effect in the visible spectral range. The demonstrated OHM platform may open up a new paradigm in nanophotonics and organic plasmonics for super‐resolution imaging and the engineering of light–matter interactions at the nanoscale.

Lee, Yeon Ui↗

High-quality microresonators in the longwave infrared based on native germanium

The longwave infrared (LWIR) region of the spectrum spans 8 to 14 μm and enables high-performance sensing and imaging for detection, ranging, and monitoring. Chip-scale LWIR photonics has enormous potential for real-time environmental monitoring, explosive detection, and biomedicine. However, realizing technologies such as precision sensors and broadband frequency combs requires ultra low-loss and low-dispersion components, which have so far remained elusive in this regime. Here, we use native germanium to demonstrate the first high-quality microresonators in the LWIR. These microresonators are coupled to partially-suspended Ge waveguides on a separate glass chip, allowing for the first unambiguous measurements of isolated linewidths. At 8 μm, we measured losses of 0.5 dB/cm and intrinsic quality (Q) factors of 2.5 × 10 5 , nearly two orders of magnitude higher than prior LWIR resonators. Our work portends the development of novel sensing and nonlinear photonics in the LWIR regime.

47 OTHER INSTRUMENTATION↗

Pressure–Modulated Luminescence Enhancement and Quenching in a Hydrogen–Bonded Organic Framework

Light emission in the solid state is central for illumination, sensing, and imaging applications. Unlike luminescence in dilute solutions, where the excited states are unimolecular in nature, intermolecular interaction plays a significant role in the quantum yield of solid-state luminophores, manifested as competing aggregation-caused quenching (ACQ) and aggregation-induced enhancement (AIE). Both effects are extensively studied in various systems; however, it remains unclear how their competition depends on molecular conformation and intermolecular stacking. Here the direct observation of pressure-modulated AIE-ACQ competition in a crystalline hydrogen-bonded organic framework (HOF) is reported. Using in situ spectroscopies and computational modeling, the intramolecular vibration and intermolecular π–π stacking directly responsible for the non-radiative decay of the excited state are identified. The extent of these two contributions is modulated by hydrostatic pressure and guest molecules in the HOF pores. Furthermore, this work demonstrates a physically neat model system to understand and control solid-state luminescence, and a potential material platform for piezoluminescent sensing.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Entangled Photon Spectroscopy

Conspectus The enhanced interest in quantum-related phenomena has provided new opportunities for chemists to push the limits of detection and analysis of chemical processes. As some have called this the second quantum revolution, a time has come to apply the rules learned from previous research in quantum phenomena toward new methods and technologies important to chemists. While there has been great interest recently in quantum information science (QIS), the quest to understand how nonclassical states of light interact with matter has been ongoing for more than two decades. Our entry into this field started around this time with the use of materials to produce nonclassical states of light. Here, the process of multiphoton absorption led to photon-number squeezed states of light, where the photon statistics are sub-Poissonian. In addition to the great interest in generating squeezed states of light, there was also interest in the formation of entangled states of light. While much of the effort is still in foundational physics, there are numerous new avenues as to how quantum entanglement can be applied to spectroscopy, imaging, and sensing. These opportunities could have a large impact on the chemical community for a broad spectrum of applications. Here, we discuss the use of entangled (or quantum) light for spectroscopy as well as applications in microscopy and interferometry. The potential benefits of the use of quantum light are discussed in detail. From the first experiments in porphyrin dendrimer systems by Dr. Dong-Ik Lee in our group to the measurements of the entangled two photon absorption cross sections of biological systems such as flavoproteins, the usefulness of entangled light for spectroscopy has been illustrated. These early measurements led the way to more advanced measurements of the unique characteristics of both entangled light and the entangled photon absorption cross-section, which provides new control knobs for manipulating excited states in molecules. The first reports of fluorescence-induced entangled processes were in organic chromophores where the entangled photon cross-section was measured. These results would later have widespread impact in applications such as entangled two-photon microscopy. From our design, construction and implementation of a quantum entangled photon excited microscope, important imaging capabilities were achieved at an unprecedented low excitation intensity of 10 7 photons/s, which is 6 orders of magnitude lower than the excitation level for the classical two-photon image. New reports have also illustrated an advantage of nonclassical light in Raman imaging as well. From a standpoint of more precise measurements, the use of entangled photons in quantum interferometry may offer new opportunities for chemistry research. Experiments that combine molecular spectroscopy and quantum interferometry, by utilizing the correlations of entangled photons in a Hong–Ou–Mandel (HOM) interferometer, have been carried out. The initial experiment showed that the HOM signal is sensitive to the presence of a resonant organic sample placed in one arm of the interferometer. In addition, parameters such as the dephasing time have been obtained with the opportunity for even more advanced phenomenology in the future.

36 MATERIALS SCIENCE↗

Strong Correlation Between Superconductivity and Ferromagnetism in an Fe-Chalcogenide Superconductor

The interplay among topology, superconductivity, and magnetism promises to bring a plethora of exotic and unintuitive behaviors in emergent quantum materials. The family of Fe-chalcogenide superconductors FeTe x Se 1–x are directly relevant in this context due to their intrinsic topological band structure, high-temperature superconductivity, and unconventional pairing symmetry. Despite enormous promise and expectation, the local magnetic properties of FeTe x Se 1–x remain largely unexplored, which prevents a comprehensive understanding of their underlying material properties. Exploiting nitrogen vacancy (NV) centers in diamond, here we report nanoscale quantum sensing and imaging of magnetic flux generated by exfoliated FeTe x Se 1–x flakes, demonstrating strong correlation between superconductivity and ferromagnetism in FeTe x Se 1–x . The coexistence of superconductivity and ferromagnetism in an established topological superconductor opens up new opportunities for exploring exotic spin and charge transport phenomena in quantum materials. The demonstrated coupling between NV centers and FeTe x Se 1–x may also find applications in developing hybrid architectures for next-generation, solid-state-based quantum information technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Layer-Dependent Magnetism and Spin Fluctuations in Atomically Thin van der Waals Magnet CrPS 4

van der Waals (vdW) magnets, an emerging family of two-dimensional (2D) materials, have received tremendous attention due to their rich fundamental physics and significant potential for cutting-edge technological applications. In contrast to the conventional bulk counterparts, vdW magnets exhibit significant tunability of local material properties, such as stacking engineered interlayer coupling and layer-number dependent magnetic and electronic interactions, which promise to deliver previously unavailable merits to develop multifunctional microelectronic devices. As a further ingredient of this emerging topic, here we report nanoscale quantum sensing and imaging of atomically thin vdW magnet chromium thiophosphate CrPS 4 , revealing its characteristic layer-dependent 2D static magnetism and dynamic spin fluctuations. We also show a large tunneling magnetoresistance in CrPS 4 -based spin filter vdW heterostructures. Here, the excellent material stability, robust strategy against environmental degradation, in combination with tailored magnetic properties highlight the potential of CrPS 4 in developing state-of-the-art 2D spintronic devices for next-generation information technologies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗