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  1. Free, publicly-accessible full text available July 1, 2023
  2. Abstract

    Nanophotonic resonators can confine light to deep-subwavelength volumes with highly enhanced near-field intensity and therefore are widely used for surface-enhanced infrared absorption spectroscopy in various molecular sensing applications. The enhanced signal is mainly contributed by molecules in photonic hot spots, which are regions of a nanophotonic structure with high-field intensity. Therefore, delivery of the majority of, if not all, analyte molecules to hot spots is crucial for fully utilizing the sensing capability of an optical sensor. However, for most optical sensors, simple and straightforward methods of introducing an aqueous analyte to the device, such as applying droplets or spin-coating, cannot achieve targeted delivery of analyte molecules to hot spots. Instead, analyte molecules are usually distributed across the entire device surface, so the majority of the molecules do not experience enhanced field intensity. Here, we present a nanophotonic sensor design with passive molecule trapping functionality. When an analyte solution droplet is introduced to the sensor surface and gradually evaporates, the device structure can effectively trap most precipitated analyte molecules in its hot spots, significantly enhancing the sensor spectral response and sensitivity performance. Specifically, our sensors produce a reflection change of a few percentage points in response to trace amounts ofmore »the amino-acid proline or glucose precipitate with a picogram-level mass, which is significantly less than the mass of a molecular monolayer covering the same measurement area. The demonstrated strategy for designing optical sensor structures may also be applied to sensing nano-particles such as exosomes, viruses, and quantum dots.

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  3. Abstract The avian transition from long to short, distally fused tails during the Mesozoic ushered in the Pygostylian group, which includes modern birds. The avian tail embodies a bipartite anatomy, with the proximal separate caudal vertebrae region, and the distal pygostyle, formed by vertebral fusion. This study investigates developmental features of the two tail domains in different bird groups, and analyzes them in reference to evolutionary origins. We first defined the early developmental boundary between the two tail halves in the chicken, then followed major developmental structures from early embryo to post-hatching stages. Differences between regions were observed in sclerotome anterior/posterior polarity and peripheral nervous system development, and these were consistent in other neognathous birds. However, in the paleognathous emu, the neognathous pattern was not observed, such that spinal nerve development extends through the pygostyle region. Disparities between the neognaths and paleognaths studied were also reflected in the morphology of their pygostyles. The ancestral long-tailed spinal nerve configuration was hypothesized from brown anole and alligator, which unexpectedly more resembles the neognathous birds. This study shows that tail anatomy is not universal in avians, and suggests several possible scenarios regarding bird evolution, including an independent paleognathous long-tailed ancestor.
  4. New trifluoromethylating reagents are designed via computational studies inspired by Togni's experimental research. Trans influence and steric effects are important for this rational design. We have found that the Togni derivative with X = SO 2 is the best choice based on its high reactivity and its potential synthesis.
  5. The RSSH + H 2 S → RSH + HSSH reaction has been suggested by numerous labs to be important in H 2 S-mediated biological processes. Seven different mechanisms for this reaction (R = CH 3 , as a model) have been studied using the DFT methods (M06-2X and ωB97X-D) with the Dunning aug-cc-pV(T+d)Z basis sets. The reaction of CH 3 SSH with gas phase H 2 S has a very high energy barrier (>45 kcal mol −1 ), consistent with the available experimental observations. A series of substitution reactions R 1 –S–S–H + − S–R 2 (R 1 = Me, t Bu, Ad, R 2 = H, S–Me, S– t Bu, S–Ad) have been studied. The regioselectivity is largely affected by the steric bulkiness of R 1 , but is much less sensitive to R 2 . Thus, when R 1 is Me, all − S–R 2 favorably attack the internal S atom, leading to R 1 –S–S–R 2 . While for R 1 = t Bu, Ad, all − S–R 2 significantly prefer to attack the external S atom to form − S–S–R 2 . These results are in good agreement with the experimental observations.