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Title: Variable-Temperature Electrospray Ionization for Temperature-Dependent Folding/Refolding Reactions of Proteins and Ligand Binding
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Publication Date:
Journal Name:
Analytical Chemistry
Page Range or eLocation-ID:
6924 to 6931
Sponsoring Org:
National Science Foundation
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  1. Abstract

    The nonnormality of temperature probability distributions and the physics that drive it are important due to their relationships to the frequency of extreme warm and cold events. Here we use a conditional mean framework to explore how horizontal temperature advection and other physical processes work together to control the shape of daily temperature distributions during 1979–2019 in the ERA5 dataset for both JJA and DJF. We demonstrate that the temperature distribution in the middle and high latitudes can largely be linearly explained by the conditional mean horizontal temperature advection with the simple treatment of other processes as a Newtonian relaxation with a spatially variant relaxation time scale and equilibrium temperature. We analyze the role of different transient and stationary components of the horizontal temperature advection in affecting the shape of temperature distributions. The anomalous advection of the stationary temperature gradient has a dominant effect in influencing temperature variance, while both that term and the covariance between anomalous wind and anomalous temperature have significant effects on temperature skewness. While this simple method works well over most of the ocean, the advection–temperature relationship is more complicated over land. We classify land regions with different advection–temperature relationships under our framework, and findmore »that for both seasons the aforementioned linear relationship can explain ∼30% of land area, and can explain either the lower or the upper half of temperature distributions in an additional ∼30% of land area. Identifying the regions where temperature advection explains shapes of temperature distributions well will help us gain more confidence in understanding the future change of temperature distributions and extreme events.

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  2. The environment experienced during embryonic development is a rich source of phenotypic variation, as environmental signals have the potential to both inform adaptive plastic responses and disrupt normal developmental programs. Environment-by-embryo interactions are particularly consequential for species with temperature-dependent sex determination, a mode of sex determination common in non-avian reptiles and fish, in which thermal cues during a discrete period of development drive the formation of either an ovary or a testis. Here we examine the impact of thermal variation during incubation in combination with developmental exposure to a common endocrine-disrupting contaminant on fitness-related hatchling traits in the American alligator (Alligator mississippiensis), a species with temperature-dependent sex determination. Using a factorial design, we exposed field-collected eggs to five thermal profiles (three constant temperatures, two fluctuating temperatures) and two environmentally relevant doses of the pesticide metabolite dichlorodiphenyldichloroethylene; and we quantified incubation duration, sex ratios, hatchling morphometric traits, and growth (9–10 days post-hatch). Whereas dichlorodiphenyldichloroethylene exposure did not generally affect hatchling traits, constant and fluctuating temperatures produced diverse phenotypic effects. Thermal fluctuations led to subtle changes in incubation duration and produced shorter hatchlings with smaller heads when compared to the constant temperature control. Warmer, male-promoting incubation temperatures resulted in larger hatchlings withmore »more residual yolk reserves when compared to cooler, female-promoting temperatures. Together, these findings advance our understanding of how complex environmental factors interact with developing organisms to generate phenotypic variation and raise questions regarding the mechanisms connecting variable thermal conditions to responses in hatchling traits and their evolutionary implications for temperature-dependent sex determination.« less
  3. Abstract. Watershed-scale stream temperature models are often one-dimensional because they require fewer data and are more computationally efficient than two- or three-dimensional models. However, one-dimensional models assume completely mixed reaches and ignore small-scale spatial temperature variability, which may create temperature barriers or refugia for cold-water aquatic species. Fine spatial- and temporal-resolution stream temperature monitoring provides information to identify river features with increased thermal variability. We used distributed temperature sensing (DTS) to observe small-scale stream temperature variability, measured as a temperature range through space and time, within two 400 m reaches in summer 2015 in Nevada's East Walker and main stem Walker rivers. Thermal infrared (TIR) aerial imagery collected in summer 2012 quantified the spatial temperature variability throughout the Walker Basin. We coupled both types of high-resolution measured data with simulated stream temperatures to corroborate model results and estimate the spatial distribution of thermal refugia for Lahontan cutthroat trout and other cold-water species. Temperature model estimates were within the DTS-measured temperature ranges 21 % and 70 % of the time for the East Walker River and main stem Walker River, respectively, and within TIR-measured temperatures 17 %, 5 %, and 5 % of the time for the East Walker, West Walker, and main stem Walker rivers, respectively. DTS, TIR, and modeledmore »stream temperatures in the main stem Walker River nearly always exceeded the 21 ∘C optimal temperature threshold for adult trout, usually exceeded the 24 ∘C stress threshold, and could exceed the 28 ∘C lethal threshold for Lahontan cutthroat trout. Measured stream temperature ranges bracketed ambient river temperatures by −10.1 to +2.3 ∘C in agricultural return flows, −1.2 to +4 ∘C at diversions, −5.1 to +2 ∘C in beaver dams, and −4.2 to 0 ∘C at seeps. To better understand the role of these river features on thermal refugia during warm time periods, the respective temperature ranges were added to simulated stream temperatures at each of the identified river features. Based on this analysis, the average distance between thermal refugia in this system was 2.8 km. While simulated stream temperatures are often too warm to support Lahontan cutthroat trout and other cold-water species, thermal refugia may exist to improve habitat connectivity and facilitate trout movement between spawning and summer habitats. Overall, high-resolution DTS and TIR measurements quantify temperature ranges of refugia and augment process-based modeling.« less