Proceedings of the National Academy of Sciences of the United States of America最新文献

{"title":"SKA2 enhances stress-related glucocorticoid receptor signaling through FKBP4–FKBP5 interactions in neurons","authors":"Jakob Hartmann, Claudia Klengel, Larissa J. Dillmann, Erin E. Hisey, Kathrin Hafner, Rammohan Shukla, Marina Soliva Estruch, Thomas Bajaj, Tim Ebert, Katharine G. Mabbott, Luise Rostin, Alexandra Philipsen, William A. Carlezon, Barbara Gisabella, Robert E. McCullumsmith, John M. Vergis, Torsten Klengel, Sabina Berretta, Nikolaos P. Daskalakis, Harry Pantazopoulos, Nils C. Gassen, Kerry J. Ressler","doi":"10.1073/pnas.2417728121","DOIUrl":"https://doi.org/10.1073/pnas.2417728121","url":null,"abstract":"Genes involved in regulating the hypothalamic–pituitary–adrenal (HPA) axis, including the glucocorticoid receptor (GR), are linked to various stress-related psychopathologies including bipolar disorder as well as other mood and trauma-related disorders. The protein product of the cell cycle gene, <jats:italic>SKA2,</jats:italic> is a GR interaction partner in peripheral cells. However, the precise roles of SKA2 in stress and GR signaling in the brain, specifically in nonreplicating postmitotic neurons, and its involvement in HPA axis regulation remain unclear. Here, we demonstrate, using diverse in vitro cell assays, a mechanism by which SKA2 promotes GR signaling through enhancing GR–FKBP4 interaction leading to dissociation of FK506-bindingprotein 51 (FKBP5) from the complex. FKBP4 and FKBP5 are cochaperones known to regulate GR function in opposite directions. Notably in mice, SKA2 in <jats:italic>Crh</jats:italic> <jats:sup>+</jats:sup> neurons of the paraventricular nucleus of the hypothalamus is crucial for HPA axis responsiveness and for maintaining the negative feedback loop underlying allostasis. Moreover, we show that SKA2 expression is increased in postmortem human hippocampus and amygdala from individuals with BD. Our study highlights a critical role of SKA2 in HPA axis function, adds to the understanding of the molecular basis of stress-related psychiatric disorders, and points to potential targets for intervention.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"89 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867593","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Permanent cilia loss during cerebellar granule cell neurogenesis involves withdrawal of cilia maintenance and centriole capping","authors":"Sandii Constable, Carolyn M. Ott, Andrew L. Lemire, Kevin White, Yu Xun, Amin Lim, Jennifer Lippincott-Schwartz, Saikat Mukhopadhyay","doi":"10.1073/pnas.2408083121","DOIUrl":"https://doi.org/10.1073/pnas.2408083121","url":null,"abstract":"Brain neurons utilize the primary cilium as a privileged compartment to detect and respond to extracellular ligands such as Sonic hedgehog (SHH). However, cilia in cerebellar granule cell (GC) neurons disassemble during differentiation through ultrastructurally unique intermediates, a process we refer to as cilia deconstruction. In addition, mature neurons do not reciliate despite having docked centrioles. Here, we identify molecular changes that accompany cilia deconstruction and centriole docking in GC neurons. We used single cell transcriptomic and immunocytological analyses to compare the transcript levels and subcellular localization of proteins between progenitor, differentiating, and mature GCs. Differentiating GCs lacked transcripts for key activators of premitotic cilia resorption, indicating that cilia disassembly in differentiating cells is distinct from premitotic cilia resorption. Instead, during differentiation, transcripts of many genes required for cilia maintenance—specifically those encoding components of intraflagellar transport, pericentrosomal material, and centriolar satellites—decreased. The abundance of several corresponding proteins in and around cilia and centrosomes also decreased. These changes coincided with downregulation of SHH signaling prior to differentiation, even in a mutant with excessive SHH activation. Finally, mother centrioles in maturing granule neurons recruited the cap complex protein, CEP97. These data suggest that a global, developmentally programmed decrease in cilium maintenance in differentiating GCs mediates cilia deconstruction, while capping of docked mother centrioles prevents cilia regrowth and dysregulated SHH signaling. Our study provides mechanistic insights expanding our understanding of permanent cilia loss in multiple tissue-specific contexts.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"83 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867588","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Capillary-driven self-assembly of soft ellipsoidal microgels at the air–water interface","authors":"Nabanita Hazra, Andrey A. Rudov, Jiarul Midya, Andrey Babenyshev, Steffen Bochenek, Martin Frenken, Walter Richtering, Gerhard Gompper, Thorsten Auth, Igor I. Potemkin, Jérôme J. Crassous","doi":"10.1073/pnas.2403690121","DOIUrl":"https://doi.org/10.1073/pnas.2403690121","url":null,"abstract":"The adsorption of ellipsoidal colloidal particles on liquid interfaces induces interfacial deformation, resulting in anisotropic interface-mediated interactions and the formation of superstructures. Soft prolate-shaped microgels at the air-water interface offer an ideal model for studying spontaneous capillary-driven self-assembly due to their tunable aspect ratio, controlled functionality, and softness. These microgels consist of a polystyrene core surrounded by a cross-linked, fluorescently labeled poly( <jats:inline-formula> <mml:math xmlns:mml=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"> <mml:mi>N</mml:mi> </mml:math> </jats:inline-formula> -isopropylmethylacrylamide) shell. By uniaxially stretching the particles embedded in polyvinyl alcohol films, the aspect ratio <jats:inline-formula> <mml:math xmlns:mml=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"> <mml:mi>ρ</mml:mi> </mml:math> </jats:inline-formula> can be finely adjusted. <jats:inline-formula> <mml:math xmlns:mml=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"> <mml:mi>ρ</mml:mi> </mml:math> </jats:inline-formula> was found to vary from 1 to 8.8 as estimated in their swollen conformation at 20 <jats:sup>°</jats:sup> C from confocal laser scanning microscopy. The spontaneous interfacial self-assembly at the air–water interface is investigated through fluorescence microscopy, theoretical calculations, and computer simulations. A structural transition occurs from a seemingly random assembly for small aspect ratios to compact clusters, which transform into a side-to-side assembly forming long chains for high aspect ratios. The influence of the poly( <jats:inline-formula> <mml:math xmlns:mml=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"> <mml:mi>N</mml:mi> </mml:math> </jats:inline-formula> -isopropylmethacrylamide) shell on the assembly indicates a significant <jats:inline-formula> <mml:math xmlns:mml=\"http://www.w3.org/1998/Math/MathML\" display=\"inline\" overflow=\"scroll\"> <mml:mi>ρ</mml:mi> </mml:math> </jats:inline-formula> -dependent microgel deformation. This deformation, in turn, determines the average distance between the particles. Consequently, capillary-driven self-assembly of soft anisotropic colloids becomes a powerful mechanism for structuring interfaces and designing microstructured materials.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"79 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867560","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Transport and energetics of bacterial rectification","authors":"Satyam Anand, Xiaolei Ma, Shuo Guo, Stefano Martiniani, Xiang Cheng","doi":"10.1073/pnas.2411608121","DOIUrl":"https://doi.org/10.1073/pnas.2411608121","url":null,"abstract":"Randomly moving active particles can be herded into directed motion by asymmetric geometric structures. Although such a rectification process has been extensively studied due to its fundamental, biological, and technological relevance, a comprehensive understanding of active matter rectification based on single particle dynamics remains elusive. Here, by combining experiments, simulations, and theory, we study the directed transport and energetics of swimming bacteria navigating through funnel-shaped obstacles—a paradigmatic model of rectification of living active matter. We develop a microscopic parameter-free model for bacterial rectification, which quantitatively explains experimental and numerical observations and predicts the optimal geometry for the maximum rectification efficiency. Furthermore, we quantify the degree of time irreversibility and measure the extractable work associated with bacterial rectification. Our study provides quantitative solutions to long-standing questions on bacterial rectification and establishes a generic relationship between time irreversibility, particle fluxes, and extractable work, shedding light on the energetics of nonequilibrium rectification processes in living systems.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"62 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867597","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Artificial dynamic structure ensemble-guided rational design of a universal RNA aptamer–based sensing tag","authors":"Jianing Hou, Pei Guo, Junyan Wang, Da Han, Weihong Tan","doi":"10.1073/pnas.2414793121","DOIUrl":"https://doi.org/10.1073/pnas.2414793121","url":null,"abstract":"Artificially functional RNAs, such as fluorogenic RNA aptamer (FRApt)-based biosensing tag, represent significant advancements in various biological applications but are limited by the lack of insight into dynamic structure ensembles and universal design concepts. Through the development of an artificial RNA structure ensemble, we rationally established an RNA reconstitution model, “SSPepper-Apt,” to generate a universal fluorogenic RNA biosensing tag. By utilizing various target-recognizing RNA motifs, SSPepper-Apt enables the modular generation of sensing tags for low-background, highly selective imaging of metabolites, peptides, and proteins in living cells. Additionally, by employing single guide RNA (sgRNA) as the recognition RNA motif, SSPepper-Apt generates fluorescence in both CRISPR-mediated imaging and gene editing only when the Cas9–sgRNA complex is successfully assembled; therefore, it can be an effective sgRNA screening tool for gene editing. Our fluorogenic RNA-sensing tag provides a universal approach for constructing functional RNA systems, avoiding the laborious and time-consuming process of sequence combination, and expanding the application of synthetic biological tools.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"111 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"MINFLUX fluorescence nanoscopy in biological tissue","authors":"Thea Moosmayer, Kamila A. Kiszka, Volker Westphal, Jasmin K. Pape, Marcel Leutenegger, Heinz Steffens, Seth G. N. Grant, Steffen J. Sahl, Stefan W. Hell","doi":"10.1073/pnas.2422020121","DOIUrl":"https://doi.org/10.1073/pnas.2422020121","url":null,"abstract":"Optical imaging access to nanometer-level protein distributions in intact tissue is a highly sought-after goal, as it would provide visualization in physiologically relevant contexts. Under the unfavorable signal-to-background conditions of increased absorption and scattering of the excitation and fluorescence light in the complex tissue sample, superresolution fluorescence microscopy methods are severely challenged in attaining precise localization of molecules. We reasoned that the typical use of a confocal detection pinhole in MINFLUX nanoscopy, suppressing background and providing optical sectioning, should facilitate the detection and resolution of single fluorophores even amid scattering and optically challenging tissue environments. Here, we investigated the performance of MINFLUX imaging for different synaptic targets and fluorescent labels in tissue sections of the mouse brain. Single fluorophores were localized with a precision of &lt;5 nm at up to 80 µm sample depth. MINFLUX imaging in two color channels allowed to probe PSD95 localization relative to the spine head morphology, while also visualizing presynaptic vesicular glutamate transporter (VGlut) 1 clustering and α-amino-3-hydroxy-5-methyl-4-isoxazolepropionic acid receptor (AMPAR) clustering at the postsynapse. Our two-dimensional (2D) and three-dimensional (3D) two-color MINFLUX results in tissue, with &lt;10 nm 3D fluorophore localization, open up broad avenues to investigate protein distributions on the single-synapse level in fixed and living brain slices.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"48 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867591","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A structure-based mechanism for initiation of AP-3 coated vesicle formation","authors":"Matthew Begley, Mahira Aragon, Richard W. Baker","doi":"10.1073/pnas.2411974121","DOIUrl":"https://doi.org/10.1073/pnas.2411974121","url":null,"abstract":"Adaptor protein complex-3 (AP-3) mediates cargo sorting from endosomes to lysosomes and lysosome-related organelles. Recently, it was shown that AP-3 adopts a constitutively open conformation compared to the related AP-1 and AP-2 coat complexes, which are inactive until undergoing large conformational changes upon membrane recruitment. How AP-3 is regulated is therefore an open question. To understand the mechanism of AP-3 membrane recruitment and activation, we reconstituted human AP-3 and determined multiple structures in the soluble and membrane-bound states using electron cryo-microscopy. Similar to yeast AP-3, human AP-3 is in a constitutively open conformation. To reconstitute AP-3 activation by adenosine di-phosphate (ADP)-ribosylation factor 1 (Arf1), a small guanosine tri-phosphate (GTP)ase, we used lipid nanodiscs to build Arf1-AP-3 complexes on membranes and determined three structures showing the stepwise conformational changes required for formation of AP-3 coated vesicles. First, membrane recruitment is driven by one of two predicted Arf1 binding sites, which flexibly tethers AP-3 to the membrane. Second, cargo binding causes AP-3 to adopt a fixed position and rigidifies the complex, which stabilizes binding for a second Arf1 molecule. Finally, binding of the second Arf1 molecule provides the template for AP-3 dimerization, providing a glimpse into the first step of coat polymerization. We propose coat polymerization only occurs after cargo engagement, thereby linking cargo sorting with assembly of higher-order coat structures. Additionally, we provide evidence for two amphipathic helices in AP-3, suggesting that AP-3 contributes to membrane deformation during coat assembly. In total, these data provide evidence for the first stages of AP-3-mediated vesicle coat assembly.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"11 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867559","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Repeated global adaptation across plant species","authors":"Gabriele Nocchi, James R. Whiting, Samuel Yeaman","doi":"10.1073/pnas.2406832121","DOIUrl":"https://doi.org/10.1073/pnas.2406832121","url":null,"abstract":"Global adaptation occurs when all populations of a species undergo selection toward a common optimum. This can occur by a hard selective sweep with the emergence of a new globally advantageous allele that spreads throughout a species’ natural range until reaching fixation. This evolutionary process leaves a temporary trace in the region affected, which is detectable using population genomic methods. While selective sweeps have been identified in many species, there have been few comparative and systematic studies of the genes involved in global adaptation. Building upon recent findings showing repeated genetic basis of local adaptation across independent populations and species, we asked whether certain genes play a more significant role in driving global adaptation across plant species. To address this question, we scanned the genomes of 17 plant species to identify signals of repeated global selective sweeps. Despite the substantial evolutionary distance between the species analyzed, we identified several gene families with strong evidence of repeated positive selection. These gene families tend to be enriched for reduced pleiotropy, consistent with predictions from Fisher’s evolutionary model and the cost of complexity hypothesis. We also found that genes with repeated sweeps exhibit elevated levels of gene duplication. Our findings contrast with recent observations of increased pleiotropy in genes driving local adaptation, consistent with predictions based on the theory of migration-selection balance.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"39 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142867562","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Growth hormone receptor in VGLUT2 or Sim1 cells regulates glycemia and insulin sensitivity","authors":"Mariana R. Tavares, Willian O. dos Santos, Andressa G. Amaral, Edward O. List, John J. Kopchick, Guilherme A. Alves, Renata Frazao, Jessica D. M. dos Santos, Alessandra G. Cruz, João Paulo Camporez, Jose Donato","doi":"10.1073/pnas.2407225121","DOIUrl":"https://doi.org/10.1073/pnas.2407225121","url":null,"abstract":"Growth hormone (GH) has several metabolic effects, including a profound impact on glucose homeostasis. For example, GH oversecretion induces insulin resistance and increases the risk of developing diabetes mellitus. Here, we show that GH receptor (GHR) ablation in vesicular glutamate transporter 2 (VGLUT2)-expressing cells, which comprise a subgroup of glutamatergic neurons, led to a slight decrease in lean body mass without inducing changes in body adiposity. VGLUT2 <jats:sup>∆GHR</jats:sup> mice exhibited reduced glycemia and improved glucose tolerance and insulin sensitivity. Among different glutamatergic neuronal populations, we found that GHR inactivation in Sim1-expressing cells recapitulated the phenotype observed in VGLUT2 <jats:sup>∆GHR</jats:sup> mice. Furthermore, Sim1 <jats:sup>∆GHR</jats:sup> mice exhibited reduced endogenous glucose production and improved hepatic insulin sensitivity without alterations in whole-body or muscle glucose uptake. Sim1 <jats:sup>∆GHR</jats:sup> mice were protected against acute but not chronic diabetogenic effects of exogenous GH administration. Pharmacological activation of ATP-sensitive potassium channels in the brain normalized blood glucose levels in Sim1 <jats:sup>∆GHR</jats:sup> mice. In conclusion, the absence of GHR signaling in VGLUT2/Sim1-expressing cells causes a persistent reduction in glycemia and improves hepatic insulin sensitivity. Central glucose-sensing mechanisms are likely involved in the reduced glycemia exhibited by Sim1 <jats:sup>∆GHR</jats:sup> mice. The current findings uncover a mechanism involved in the effects of GHR signaling in regulating glucose homeostasis.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"14 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858535","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Lanthanide binding peptide surfactants at air–aqueous interfaces for interfacial separation of rare earth elements","authors":"Luis E. Ortuno Macias, Felipe Jiménez-Ángeles, Jason G. Marmorstein, Yiming Wang, Stephen A. Crane, Surabh K. T., Pan Sun, Bikash Sapkota, Eshe Hummingbird, Woojin Jung, Baofu Qiao, Daeyeon Lee, Ivan J. Dmochowski, Robert J. Messinger, Mark L. Schlossman, Cesar de la Fuente-Nunez, Ravi Radhakrishnan, E. James Petersson, Monica Olvera de la Cruz, Wei Bu, Mrinal Bera, Binhua Lin, Raymond S. Tu, Kathleen J. Stebe, Charles Maldarelli","doi":"10.1073/pnas.2411763121","DOIUrl":"https://doi.org/10.1073/pnas.2411763121","url":null,"abstract":"Rare earth elements (REEs) are critical materials to modern technologies. They are obtained by selective separation from mining feedstocks consisting of mixtures of their trivalent cation. We are developing an all-aqueous, bioinspired, interfacial separation using peptides as amphiphilic molecular extractants. Lanthanide binding tags (LBTs) are amphiphilic peptide sequences based on the EF-hand metal binding loops of calcium-binding proteins which complex selectively REEs. We study LBTs optimized for coordination to Tb <jats:sup>3+</jats:sup> using luminescence spectroscopy, surface tensiometry, X-ray reflectivity, and X-ray fluorescence near total reflection, and find that these LBTs capture Tb <jats:sup>3+</jats:sup> in bulk and adsorb the complex to the interface. Molecular dynamics show that the binding pocket remains intact upon adsorption. We find that, if the net negative charge on the peptide results in a negatively charged complex, excess cations are recruited to the interface by nonselective Coulombic interactions that compromise selective REE capture. If, however, the net negative charge on the peptide is −3, resulting in a neutral complex, a 1:1 surface ratio of cation to peptide is achieved. Surface adsorption of the neutral peptide complexes from an equimolar mixture of Tb <jats:sup>3+</jats:sup> and La <jats:sup>3+</jats:sup> demonstrates a switchable platform dictated by bulk and interfacial effects. The adsorption layer becomes enriched in the favored Tb <jats:sup>3+</jats:sup> when the bulk peptide is saturated, but selective to La <jats:sup>3+</jats:sup> for undersaturation due to a higher surface activity of the La <jats:sup>3+</jats:sup> complex.","PeriodicalId":20548,"journal":{"name":"Proceedings of the National Academy of Sciences of the United States of America","volume":"1 1","pages":""},"PeriodicalIF":11.1,"publicationDate":"2024-12-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142858537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"综合性期刊","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}