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Cobalt-Salen Catalyzed Electroreductive Alkylation of Activated Olefins
Laboratoire Synthèse Electrochimie Imagerie et Systèmes Analytiques - Sylvie Condon , Céline Cannes , and Fethi Bedioui
Journal of Chemistry - - doi.org/10.1155/2019/9832639 - 2019
Cobalt-Salen mediated electroreductive and regioselective alkylation of electron deficient olefins is reported in one step in an undivided electrochemical cell, in the presence of an iron rod as sacrificial anode. Although the reactivity depends on the class of alkyl halides, the reported study offers a green and expeditious electrosynthetic route for Csp3-Csp3 bond formation in mild conditions. This study also confirms the possible formation of the heterobinuclear cobalt-Salen-iron complex previously reported as the effective catalyst.
Phase separations, liquid crystal ordering and molecular partitioning in mixtures of PEG and DNA oligomers
LABORATOIRE AUTO-ASSEMBLAGE MOLÉCULAIRE - Simone Di Leo, Marco Todisco, Tommaso Bellini, Tommaso P. Fraccia
Molecular Crystals and Liquid Crystals - - DOI: 10.1080/02678292.2018.1519123 - 2018
Liquid crystals (LCs) ordering of DNA and RNA oligomers relies on the presence of inter-duplex end-to-end attraction, driving the formation of linear aggregates. Such interactions are gauged, at a macroscopic level, by the osmotic pressure at the isotropic-nematic and nematic-columnar phase transitions. We studied aqueous solutions of PEG and DNA duplex-forming oligomers, finding that there is a wide range of concentrations in which these mixtures phase separate into coexisting PEG-rich and DNA-rich phases, the latter being either in the isotropic state or ordered as a nematic or columnar LC. We determined the phase diagram in mixtures of PEG and DNA duplexes with different terminal motifs – blunt ends, sticky overhangs, aggregation-preventing overhangs – and measured the partitioning of the species in the coexisting phases. On this basis, we determined the osmotic pressure as a function of the DNA concentration across the phase diagram. We compared the equation of state obtained in this way with both the Carnahan–Starling equation of state for hard spheres and with the pressure predicted by computer simulations of a system of aggregating cylinders. We obtain a good agreement between experiments and simulations, and end-to-end attraction energies of the order of 6 kcal/mol, a bit larger than expected, but still in agreement with the current models for DNA-DNA interactions.
Phase separations, liquid crystal ordering and molecular partitioning in mixtures of PEG and DNA oligomers
LABORATOIRE AUTO-ASSEMBLAGE MOLÉCULAIRE - Simone Di Leo, Marco Todisco, Tommaso Bellini, Tommaso P. Fraccia
Molecular Crystals and Liquid Crystals - - DOI: 10.1080/02678292.2018.1519123 - 2018
Liquid crystals (LCs) ordering of DNA and RNA oligomers relies on the presence of inter-duplex end-to-end attraction, driving the formation of linear aggregates. Such interactions are gauged, at a macroscopic level, by the osmotic pressure at the isotropic-nematic and nematic-columnar phase transitions. We studied aqueous solutions of PEG and DNA duplex-forming oligomers, finding that there is a wide range of concentrations in which these mixtures phase separate into coexisting PEG-rich and DNA-rich phases, the latter being either in the isotropic state or ordered as a nematic or columnar LC. We determined the phase diagram in mixtures of PEG and DNA duplexes with different terminal motifs – blunt ends, sticky overhangs, aggregation-preventing overhangs – and measured the partitioning of the species in the coexisting phases. On this basis, we determined the osmotic pressure as a function of the DNA concentration across the phase diagram. We compared the equation of state obtained in this way with both the Carnahan–Starling equation of state for hard spheres and with the pressure predicted by computer simulations of a system of aggregating cylinders. We obtain a good agreement between experiments and simulations, and end-to-end attraction energies of the order of 6 kcal/mol, a bit larger than expected, but still in agreement with the current models for DNA-DNA interactions.
Nonenzymatic Polymerization into Long Linear RNA Templated by Liquid Crystal Self-Assembly
LABORATOIRE AUTO-ASSEMBLAGE MOLÉCULAIRE - Marco Todisco Tommaso Pietro Fraccia Greg P. Smith Andrea Corno
ACS Nano - 12(10) - DOI: 10.1021/acsnano.8b05821 - 2018
Self-synthesizing materials, in which supramolecular structuring enhances the formation of new molecules that participate to the process, represent an intriguing notion to account for the first appearance of biomolecules in an abiotic Earth. We present here a study of the abiotic formation of interchain phosphodiester bonds in solutions of short RNA oligomers in various states of supramolecular arrangement and their reaction kinetics. We found a spectrum of conditions in which RNA oligomers self-assemble and phase separate into highly concentrated ordered fluid liquid crystal (LC) microdomains. We show that such supramolecular state provides a template guiding their ligation into hundred-bases long chains. The quantitative analysis presented here demonstrates that nucleic acid LC boosts the rate of end-to-end ligation and suppresses the formation of the otherwise dominant cyclic oligomers. These results strengthen the concept of supramolecular ordering as an efficient pathway toward the emergence of the RNA World in the primordial Earth.
Backbone-free duplex-stacked monomer nucleic acids exhibiting Watson-Crick selectivity
LABORATOIRE AUTO-ASSEMBLAGE MOLÉCULAIRE - Gregory P Smith , Tommaso P Fraccia , Marco Todisco , Giuliano Zanchetta , Chenhui Zhu , Emily Hayden , Tommaso Bellini , Noel A Clark
ACS Nano - 115(33) E7658-E7664 - DOI: 10.1073/pnas.1721369115 - 2018
We demonstrate that nucleic acid (NA) mononucleotide triphosphates (dNTPs and rNTPs), at sufficiently high concentration and low temperature in aqueous solution, can exhibit a phase transition in which chromonic columnar liquid crystal ordering spontaneously appears. Remarkably, this polymer-free state exhibits, in a self-assembly of NA monomers, the key structural elements of biological nucleic acids, including: long-ranged duplex stacking of base pairs, complementarity-dependent partitioning of molecules, and Watson-Crick selectivity, such that, among all solutions of adenosine, cytosine, guanine, and thymine NTPs and their binary mixtures, duplex columnar ordering is most stable in the A-T and C-G combinations.
Liquid Crystal Ordering of Four-Base-Long DNA Oligomers with Both G–C and A–T Pairing
LABORATOIRE AUTO-ASSEMBLAGE MOLÉCULAIRE - Tommaso P. Fraccia , Gregory P. Smith , Noel A. Clark and Tommaso Bellini
CRYSTALS - 8(1) 5 - doi.org/10.3390/cryst8010005 - 2018
We report the liquid crystal (LC) ordering in an aqueous solution of four-base-long DNA oligomers 50-GCTA-30. In such systems, the formation of the chiral nematic (N*) LC phase is the result of a continuous self-assembly process in which double helix stability is achieved only through linear chaining of multiple DNA strands. The thermal stability of the aggregates and their LC phase diagram have been experimentally investigated, quantitatively interpreted with theoretical models and compared with recent results on four-base sequences with only G–C or only A–T pairing motifs. N* phase is found at GCTA concentration, cDNA, between 240 and 480 mg/mL and at temperature T < 30 C. The twist of the nematic director is found to be left-handed with pitch (p) in the optical range, increasing with cDNA and decreasing with T.
Sign epistasis caused by hierarchy within signalling cascades.
Laboratoire Biochimie - Nghe P, Kogenaru M, Tans SJ.
Nat Commun - 9(1) 1451. - doi: 10.1038/s41467-018-03644-8 - 2018
Sign epistasis is a central evolutionary constraint, but its causal factors remain difficult to predict. Here we use the notion of parameterised optima to explain epistasis within a signalling cascade, and test these predictions in Escherichia coli. We show that sign epistasis arises from the benefit of tuning phenotypic parameters of cascade genes with respect to each other, rather than from their complex and incompletely known genetic bases. Specifically, sign epistasis requires only that the optimal phenotypic parameters of one gene depend on the phenotypic parameters of another, independent of other details, such as activating or repressing nature, position within the cascade, intra-genic pleiotropy or genotype. Mutational effects change sign more readily in downstream genes, indicating that optimising downstream genes is more constrained. The findings show that sign epistasis results from the inherent upstream-downstream hierarchy between signalling cascade genes, and can be addressed without exhaustive genotypic mapping.
Coupled catabolism and anabolism in autocatalytic RNA sets.
Laboratoire Biochimie - Arsène S, Ameta S, Lehman N, Griffiths AD, Nghe P.
Nucleic Acids Res. - 46(18) 9660-9666 - doi: 10.1093/nar/gky598. - 2018
The ability to process molecules available in the environment into useable building blocks characterizes catabolism in contemporary cells and was probably critical for the initiation of life. Here we show that a catabolic process in collectively autocatalytic sets of RNAs allows diversified substrates to be assimilated. We modify fragments of the Azoarcus group I intron and find that the system is able to restore the original native fragments by a multi-step reaction pathway. This allows in turn the formation of catalysts by an anabolic process, eventually leading to the accumulation of ribozymes. These results demonstrate that rudimentary self-reproducing RNA systems based on recombination possess an inherent capacity to assimilate an expanded repertoire of chemical resources and suggest that coupled catabolism and anabolism could have arisen at a very early stage in primordial living systems.
Selection Dynamics in Transient Compartmentalization.
Laboratoire Biochimie - Blokhuis A, Lacoste D, Nghe P, Peliti L
Phys. Rev. Lett. - 158101 120(15): - doi: 10.1371/journal.pcbi.1004972 - 2018
Transient compartments have been recently shown to be able to maintain functional replicators in the context of prebiotic studies. Here, we show that a broad class of selection dynamics is able to achieve this goal. We identify two key parameters, the relative amplification of nonactive replicators (parasites) and the size of compartments. These parameters account for competition and diversity, and the results are relevant to similar multilevel selection problems, such as those found in virus-host ecology and trait group selection.
Selection Dynamics in Transient Compartmentalization
Laboratoire Biochimie - doi.org/10.1103/PhysRevLett.120.158101
Phys. Rev. Lett. - 120 158101 - doi.org/10.1103/PhysRevLett.120.158101 - 2018
Transient compartments have been recently shown to be able to maintain functional replicators in the context of prebiotic studies. Here, we show that a broad class of selection dynamics is able to achieve this goal. We identify two key parameters, the relative amplification of nonactive replicators (parasites) and the size of compartments. These parameters account for competition and diversity, and the results are relevant to similar multilevel selection problems, such as those found in virus-host ecology and trait group selection.
Spontaneous migration of cellular aggregates from giant keratocytes to running spheroids.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Grégory Beaune, Carles Blanch-Mercader, Stéphane Douezan, Julien Dumond, David Gonzalez-Rodriguez, Damien Cuvelier, Thierry Ondarçuhu, Pierre Sens, Sylvie Dufour, Michael P Murrell, Françoise Brochard-Wyart
Proceedings of the National Academy of Sciences of the United States of America - 12926-12931 - 10.1073/pnas.1811348115 - 2018
Despite extensive knowledge on the mechanisms that drive single-cell migration, those governing the migration of cell clusters, as occurring during embryonic development and cancer metastasis, remain poorly understood. Here, we investigate the collective migration of cell on adhesive gels with variable rigidity, using 3D cellular aggregates as a model system. After initial adhesion to the substrate, aggregates spread by expanding outward a cell monolayer, whose dynamics is optimal in a narrow range of rigidities. Fast expansion gives rise to the accumulation of mechanical tension that leads to the rupture of cell-cell contacts and the nucleation of holes within the monolayer, which becomes unstable and undergoes dewetting like a liquid film. This leads to a symmetry breaking and causes the entire aggregate to move as a single entity. Varying the substrate rigidity modulates the extent of dewetting and induces different modes of aggregate motion: « giant keratocytes, » where the lamellipodium is a cell monolayer that expands at the front and retracts at the back; « penguins, » characterized by bipedal locomotion; and « running spheroids, » for nonspreading aggregates. We characterize these diverse modes of collective migration by quantifying the flows and forces that drive them, and we unveil the fundamental physical principles that govern these behaviors, which underscore the biological predisposition of living material to migrate, independent of length scale.
Innate Immune Signals Induce Anterograde Endosome Transport Promoting MHC Class I Cross-Presentation.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Weimershaus M, Mauvais FX, Saveanu L, Adiko C, Babdor J, Abramova A, Montealegre S, Lawand M, Evnouchidou I, Huber KJ, Chadt A, Zwick M, Vargas P, Dussiot M, Lennon-Dumenil AM, Brocker T, Al-Hasani H, van Endert P.
Cell Reports - 24(13) 3568-3581 - doi: 10.1016/j.celrep.2018.08.041 - 2018
Both cross-presentation of antigens by dendritic cells, a key pathway triggering T cell immunity and immune tolerance, and survival of several pathogens residing in intracellular vacuoles are intimately linked to delayed maturation of vesicles containing internalized antigens and microbes. However, how early endosome or phagosome identity is maintained is incompletely understood. We show that Toll-like receptor 4 (TLR4) and Fc receptor ligation induces interaction of the GTPase Rab14 with the kinesin KIF16b mediating plus-end-directed microtubule transport of endosomes. As a result, Rab14 recruitment to phagosomes delays their maturation and killing of an internalized pathogen. Enhancing anterograde transport by overexpressing Rab14, promoting the GTP-bound Rab14 state, or inhibiting retrograde transport upregulates cross-presentation. Conversely, reducing Rab14 expression, destabilizing Rab14 endosomes, and inhibiting anterograde microtubule transport by Kif16b knockdown compromise cross-presentation. Therefore, regulation of early endosome trafficking by innate immune signals is a critical parameter in cross-presentation by dendritic cells.
Diversification of human plasmacytoid predendritic cells in response to a single stimulus
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Alculumbre SG, Saint-André V1, Di Domizio J, Vargas P, Sirven P, Bost P, Maurin M, Maiuri P, Wery M, Roman MS, Savey L, Touzot M, Terrier B, Saadoun D, Conrad C, Gilliet M, Morillon A, Soumelis V.
Nat Immunol. - 19(1) 63-75 - doi: 10.1038/s41590-017-0012-z - 2018
Innate immune cells adjust to microbial and inflammatory stimuli through a process termed environmental plasticity, which links a given individual stimulus to a unique activated state. Here, we report that activation of human plasmacytoid predendritic cells (pDCs) with a single microbial or cytokine stimulus triggers cell diversification into three stable subpopulations (P1-P3). P1-pDCs (PD-L1+CD80-) displayed a plasmacytoid morphology and specialization for type I interferon production. P3-pDCs (PD-L1-CD80+) adopted a dendritic morphology and adaptive immune functions. P2-pDCs (PD-L1+CD80+) displayed both innate and adaptive functions. Each subpopulation expressed a specific coding- and long-noncoding-RNA signature and was stable after secondary stimulation. P1-pDCs were detected in samples from patients with lupus or psoriasis. pDC diversification was independent of cell divisions or preexisting heterogeneity within steady-state pDCs but was controlled by a TNF autocrine and/or paracrine communication loop. Our findings reveal a novel mechanism for diversity and division of labor in innate immune cells.
Spontaneous migration of cellular aggregates from giant keratocytes to running spheroids
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Grégory Beaune, Carles Blanch-Mercader, Stéphane Douezan, Julien Dumond, David Gonzalez-Rodriguez, Damien Cuvelier, Thierry Ondarçuhu, Pierre Sens, Sylvie Dufour, Michael P. Murrell, and Françoise Brochard-Wyart
Cell Sci - 115 (51) 12926-12931 - doi.org/10.1073/pnas.1811348115 - 2018
Despite extensive knowledge on the mechanisms that drive single-cell migration, those governing the migration of cell clusters, as occurring during embryonic development and cancer metastasis, remain poorly understood. Here, we investigate the collective migration of cell on adhesive gels with variable rigidity, using 3D cellular aggregates as a model system. After initial adhesion to the substrate, aggregates spread by expanding outward a cell monolayer, whose dynamics is optimal in a narrow range of rigidities. Fast expansion gives rise to the accumulation of mechanical tension that leads to the rupture of cell–cell contacts and the nucleation of holes within the monolayer, which becomes unstable and undergoes dewetting like a liquid film. This leads to a symmetry breaking and causes the entire aggregate to move as a single entity. Varying the substrate rigidity modulates the extent of dewetting and induces different modes of aggregate motion: “giant keratocytes,” where the lamellipodium is a cell monolayer that expands at the front and retracts at the back; “penguins,” characterized by bipedal locomotion; and “running spheroids,” for nonspreading aggregates. We characterize these diverse modes of collective migration by quantifying the flows and forces that drive them, and we unveil the fundamental physical principles that govern these behaviors, which underscore the biological predisposition of living material to migrate, independent of length scale.
Adhesion to nanofibers drives cell membrane remodeling through one-dimensional wetting.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Arthur Charles-Orszag, Feng-Ching Tsai, Daria Bonazzi, Valeria Manriquez, Martin Sachse, Adeline Mallet, Audrey Salles, Keira Melican, Ralitza Staneva, Aurélie Bertin, Corinne Millien, Sylvie Goussard, Pierre Lafaye, Spencer Shorte, Matthieu Piel, Jacomi
Nature Communications - 185.41666667 - Adhesion to nanofibers drives cell membrane remodeling through one-dimensional wetting. - 2018
The shape of cellular membranes is highly regulated by a set of conserved mechanisms that can be manipulated by bacterial pathogens to infect cells. Remodeling of the plasma membrane of endothelial cells by the bacterium Neisseria meningitidis is thought to be essential during the blood phase of meningococcal infection, but the underlying mechanisms are unclear. Here we show that plasma membrane remodeling occurs independently of F-actin, along meningococcal type IV pili fibers, by a physical mechanism that we term ‘one-dimensional’ membrane wetting. We provide a theoretical model that describes the physical basis of one-dimensional wetting and show that this mechanism occurs in model membranes interacting with nanofibers, and in human cells interacting with extracellular matrix meshworks. We propose one-dimensional wetting as a new general principle driving the interaction of cells with their environment at the nanoscale that is diverted by meningococci during infection.
Size control in mammalian cells involves modulation of both growth rate and cell cycle duration.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Article | OPEN | Published: 16 August 2018 Size control in mammalian cells involves modulation of both growth rate and cell cycle duration Clotilde Cadart, Sylvain Monnier, Jacopo Grilli, Pablo J. Sáez, Nishit Srivastava, Rafaele Attia, Emmanuel Terriac
Nature Communications - 9 3275 - DOI : 10.1038/s41467-018-05393-0 - 2018
Despite decades of research, how mammalian cell size is controlled remains unclear because of the difficulty of directly measuring growth at the single-cell level. Here we report direct measurements of single-cell volumes over entire cell cycles on various mammalian cell lines and primary human cells. We find that, in a majority of cell types, the volume added across the cell cycle shows little or no correlation to cell birth size, a homeostatic behavior called “adder”. This behavior involves modulation of G1 or S-G2 duration and modulation of growth rate. The precise combination of these mechanisms depends on the cell type and the growth condition. We have developed a mathematical framework to compare size homeostasis in datasets ranging from bacteria to mammalian cells. This reveals that a near-adder behavior is the most common type of size control and highlights the importance of growth rate modulation to size control in mammalian cells.
LINC complex-Lis1 interplay controls MT1-MMP matrix digest-on-demand response for confined tumor cell migration.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Elvira Infante, Alessia Castagnino, Robin Ferrari, Pedro Monteiro, Sonia Agüera-González, Perrine Paul-Gilloteaux, Mélanie J Domingues, Paolo Maiuri, Matthew Raab, Catherine M Shanahan, Alexandre Baffet, Matthieu Piel, Edgar R Gomes, Philippe Chavrier
Nature Communications - 9 2443 - DOI : 10.1038/s41467-018-04865-7 - 2018
Cancer cells’ ability to migrate through constricting pores in the tissue matrix is limited by nuclear stiffness. MT1-MMP contributes to metastasis by widening matrix pores, facilitating confined migration. Here, we show that modulation of matrix pore size or of lamin A expression known to modulate nuclear stiffness directly impinges on levels of MT1-MMP-mediated pericellular collagenolysis by cancer cells. A component of this adaptive response is the centrosome-centered distribution of MT1-MMP intracellular storage compartments ahead of the nucleus. We further show that this response, including invadopodia formation in association with confining matrix fibrils, requires an intact connection between the nucleus and the centrosome via the linker of nucleoskeleton and cytoskeleton (LINC) complex protein nesprin-2 and dynein adaptor Lis1. Our results uncover a digest-on-demand strategy for nuclear translocation through constricted spaces whereby confined migration triggers polarization of MT1-MMP storage compartments and matrix proteolysis in front of the nucleus depending on nucleus-microtubule linkage.
Role of calcium permeable channels in dendritic cell migration.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Sáez PJ, Sáez JC, Lennon-Duménil AM, Vargas P.
Curr Opin Immunol. - 52 74-80 - doi: 10.1016/j.coi.2018.04 - 2018
Calcium ion (Ca2+) is an essential second messenger involved in multiple cellular and subcellular processes. Ca2+ can be released and sensed globally or locally within cells, providing complex signals of variable amplitudes and time-scales. The key function of Ca2+ in the regulation of acto-myosin contractility has provided a simple explanation for its role in the regulation of immune cell migration. However, many questions remain, including the identity of the Ca2+ stores, channels and upstream signals involved in this process. Here, we focus on dendritic cells (DCs), because their immune sentinel function heavily relies on their capacity to migrate within tissues and later on between tissues and lymphoid organs. Deciphering the mechanisms by which cytoplasmic Ca2+ regulate DC migration should shed light on their role in initiating and tuning immune responses.
Mixed Copolymer Adlayers Allowing Reversible Thermal Control of Single Cell Aspect Ratio.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Dalier F, Dubacheva GV, Coniel M, Zanchi D, Galtayries A, Piel M, Marie E, Tribet C.
ACS Appl Mater Interfaces - 10(3) 2253-2258 - doi: 10.1021/acsami.7b18513. - 2018
Dynamic guidance of living cells is achieved by fine-tuning and spatiotemporal modulation on artificial polymer layers enabling reversible peptide display. Adjustment of surface composition and interactions is obtained by coadsorption of mixed poly(lysine) derivatives, grafted with either repellent PEG, RGD adhesion peptides, or T-responsive poly(N-isopropylacrylamide) strands. Deposition of mixed adlayers provides a straightforward mean to optimize complex substrates, which is here implemented to achieve (1) thermal control of ligand accessibility and (2) adjustment of relative adhesiveness between adjacent micropatterns, while preserving cell attachment during thermal cycles. The reversible polarization of HeLa cells along orthogonal stripes mimics guidance along natural matrices.
Retraction Notice to: FMN2 Makes Perinuclear Actin to Protect Nuclei during Confined Migration and Promote Metastasis.
Laboratoire Biologie cellulaire systémique de la polarité et de la division - Skau CT, Fischer RS, Gurel P, Thiam HR, Tubbs A, Baird MA, Davidson MW, Piel M, Alushin GM, Nussenzweig A, Steeg PS, Waterman CM.
Cell - 173(2) 529 - doi: 10.1016/j.cell.2018.03.058 - 2018
FMN2 Makes Perinuclear Actin to Protect Nuclei during Confined Migration and Promote Metastasis. [Cell. 2016]

584 publications.