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PNAS Plus Significance Statements PNAS PLUS PNAS PLUS PNAS Plus Significance Statements Effect of material flexibility on the thermodynamics (PPAR) δ concomitant with distinct conformational and kinetics of hydrophobically induced changes in the receptor, key to therapeutic modu- evaporation of water lation of lipid catabolism, transport, and storage. Y. Elia Altabet, Amir Haji-Akbari ( ), These studies reveal the subtle interplay between li- and Pablo G. Debenedetti gand configuration and chemistry coupled to modu- δ – The evaporation of water in hydrophobic confinement lation of PPAR structural dynamics. This set of structure is important for the formation and function of both activity relationships (SARs) guide synthetic ligand natural and synthetic hydrophobic self-assemblies. designs necessary to refine therapeutic leads for δ Using advanced computational techniques, we find temporally and spatially regulating PPAR during the that the thermodynamic and kinetic stability of water course of metabolic disease onset and progression. – in hydrophobic confinement is extremely sensitive to (See pp. E2563 E2570.) the flexibility of the confining material. In the context of engineered systems, this work suggests that the Biological regulation of atmospheric chemistry mechanical properties of the building blocks in a self- en route to planetary oxygenation assembled system are a crucial design consideration. Gareth Izon, Aubrey L. Zerkle, Kenneth H. Williford, James With respect to biophysical phenomena, it suggests Farquhar, Simon W. Poulton, and Mark W. Claire that small changes in flexibility can induce switch-like It has been proposed that enhanced methane fluxes to responses such as the opening and closing of mem- Earth’s early atmosphere could have altered atmo- brane channels and the conversion between active spheric chemistry, initiating a hydrocarbon-rich haze and inactive states in receptors, both of which are reminiscent of Saturn’s moon Titan. The occurrence, – common drug targets. (See pp. E2548 E2555.) cause, and significance of haze development, how- ever, remain unknown. Here, we test and refine the Electron transfer between anatase TiO2 and “haze hypothesis” by combining an ultra-high-resolu- an O2 molecule directly observed by atomic force microscopy tion sulfur- and carbon-isotope dataset with photo- chemical simulations to reveal the structure and timing Martin Setvin, Jan Hulva, Gareth S. Parkinson, Michael of haze development. These data suggest that haze Schmid, and Ulrike Diebold persisted for ∼1 million years, requiring a sustained Molecular oxygen is an inert species, unable to enter biological driver. We propose that enhanced atmo- chemical reactions. Activation occurs through the spheric CH4, implied by the presence of haze, could acceptance of an extra electron; this catalytic step have had a significant impact on the escape of hy- plays a major role in applications such as heteroge- drogen from the atmosphere, effectively contributing neous catalysis and fuel cells. It is also used by all to the terminal oxidation of Earth’s surficial environ- living organisms. We show that the two different ments ∼2.4 billion years ago. (See pp. E2571–E2579.) charge states of O2 can be easily distinguished by atomic force microscopy (AFM). We directly injected Optimal run-and-tumble–based transportation or removed electrons into/from the O2 molecule by of a Janus particle with active steering the AFM tip, switching the O reactivity. These results 2 Tomoyuki Mano, Jean-Baptiste Delfau, Junichiro Iwasawa, open new possibilities for studying catalytic and and Masaki Sano photocatalytic processes. (See pp. E2556–E2562.) Commanding the swimming of micrometric objects Structural basis for specific ligation of the subjected to thermal agitation is always challenging for peroxisome proliferator-activated receptor δ both artificial and living systems. Now, artificial swim- Chyuan-Chuan Wu, Thomas J. Baiga, Michael Downes, mers can be designed with self-propelling force that James J. La Clair, Annette R. Atkins, Stephane B. Richard, can be tuned at will. However, orienting such small Weiwei Fan, Theresa A. Stockley-Noel, Marianne E. Bowman, particles to an arbitrary direction requires counter- Joseph P. Noel, and Ronald M. Evans balancing the random rotational diffusion. Here, we Clinical treatments for metabolic diseases rely on introduce a simple concept to reorient artificial swim- agents with high selectivity to specific targets often mers, granting them a motion similar to the run-and- within a class of structurally and functionally related tumbling behavior of Escherichia coli.Weshowitusing proteins. In this paper, we uncover physical and chem- Janus particles with asymmetric surface coating and ical features governing selective small-molecule bind- moving under an ac electric field. Moreover, we de- ing to peroxisome proliferator-activated receptor termine the optimal strategy and compare it with 3292–3296 | PNAS | March 28, 2017 | vol. 114 | no. 13 www.pnas.org/cgi/doi/10.1073/pnas.ss11413 Downloaded by guest on September 27, 2021 biological swimmers. Our results encourage additional in- instead the resulting photoproduct is thermally reisomerized back vestigation into dynamical behavior of colloidal particles as to its inactive state, abrogating the necessity for a complex reti- well as application to microscopic devices. (See pp. E2580–E2589.) noid cycle to renew its chromophore. This photocyclic behavior of Rh6mr opens up several avenues for using optogenetic tools Cross-cousin marriage among the Yanomamö shows based on vertebrate Rhs. (See pp. E2608–E2615.) evidence of parent–offspring conflict and mate competition between brothers Phytosphingosine degradation pathway includes fatty acid α Napoleon A. Chagnon, Robert F. Lynch, Mary K. Shenk, Raymond Hames, -oxidation reactions in the endoplasmic reticulum and Mark V. Flinn Takuya Kitamura, Naoya Seki, and Akio Kihara Cross-cousin marriage (i.e., marriage with the offspring of a par- Although the synthetic pathway of phytosphingosine is already ent’s opposite-sex sibling) is the most common preferred mar- known, its degradation pathway has remained unclear. In the riage arrangement across cultures. Despite intense investigation, present study, we reveal the entire phytosphingosine degrada- the origin and adaptive function of this marriage prescription tion pathway, where fatty acid α-oxidation is involved. We show have not been resolved. An analysis of the fitness consequences that the Sjögren–Larsson syndrome-causative gene ALDH3A2 of marriages in the Yanomamö—a tribal society in the Amazon— and HACL2 (2-hydroxyacyl-CoA lyase 2) are involved in the fatty shows that parents and brothers achieve higher fitness outcomes acid α-oxidation reactions as an aldehyde dehydrogenase and a when their respective children and sisters marry more closely 2-hydroxy acyl-CoA lyase, respectively. Our findings are impor- related individuals. Meanwhile, the spouses and offspring pro- tant for understanding the molecular mechanism of phytos- duced by these unions have lower fitness. These findings suggest phingosine/sphingolipid homeostasis. HACL2 is localized in the that cross-cousin marriage prescriptions and taboos against endoplasmic reticulum, indicating that fatty acid α-oxidation oc- marrying parallel cousins owe their origin to parent–offspring curs in the endoplasmic reticulum in mammals, in addition to the conflict through parental control of marriage and competition α-oxidation already known to occur in peroxisomes. (See pp. between same-sex siblings. (See pp. E2590–E2597.) E2616–E2623.) Morphological features of IFN-γ–stimulated mesenchymal Structure-guided SCHEMA recombination generates stromal cells predict overall immunosuppressive capacity diverse chimeric channelrhodopsins Matthew W. Klinker, Ross A. Marklein, Jessica L. Lo Surdo, Cheng-Hong Claire N. Bedbrook, Austin J. Rice, Kevin K. Yang, Xiaozhe Ding, Siyuan Wei, and Steven R. Bauer Chen, Emily M. LeProust, Viviana Gradinaru, and Frances H. Arnold Substantial evidence exists demonstrating the immunosup- Critical for regulating cell function, integral membrane proteins pressive function of mesenchymal stromal cells (MSCs), but in- (MPs) are key engineering targets. MP engineering is limited consistent clinical results suggest that better understanding of because these proteins are difficult to express with proper plasma MSC-mediated immunosuppression and identification of fea- membrane localization in heterologous systems. We investigate tures predictive of immunosuppressive capacity would advance the expression, localization, and light-induced behavior of the MSC-based therapeutics. In this work, we present a robust an- light-gated MP channel, channelrhodopsin (ChR), because of its alytical approach to quantify the immunosuppressive capacity utility in studying neuronal circuitry. We used structure-guided of MSCs by integrating high-dimensional flow cytometry data SCHEMA recombination to generate libraries of chimeric ChRs from multiple experimental conditions into a single measure of that are diverse in sequence yet still capable of efficient ex- immunosuppressive capacity. Additionally, we identified mor- pression, localization, and useful light-induced functionality. phological features of MSCs that predicted immunosuppressive The conservative nature of recombination generates unique capacity, as well as the magnitude of IFN-γ–mediated immuno- protein sequences that tend to fold and function. Recombination is suppression enhancement. These
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