{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,15]],"date-time":"2026-09-15T15:52:45Z","timestamp":1789487565739,"version":"build-2803163510"},"reference-count":38,"publisher":"American Chemical Society (ACS)","issue":"36","license":[{"start":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T00:00:00Z","timestamp":1786924800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by-nc-nd\/4.0\/"}],"funder":[{"DOI":"10.13039\/100000006","name":"Office of Naval Research","doi-asserted-by":"publisher","award":["MURI N00014-23-1-2499"],"award-info":[{"award-number":["MURI N00014-23-1-2499"]}],"id":[{"id":"10.13039\/100000006","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,9,15]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Understanding how molecular-scale interactions govern the assembly and processing of nanocomposite tectons (NCTs) is essential for the design of functional nanoparticle superlattices. Here, we present a multiscale simulation framework that connects explicit microscale descriptions of polymer-grafted, supramolecularly functionalized NCTs to mesoscale predictions of superlattice formation and cold sintering. Potentials of mean force (PMFs) extracted from microscale simulations show that the graft length and nanoparticle diameter tune both the depth and range of effective attraction through the interplay of hydrogen bond-mediated association, brush entropy, and core curvature. These interactions predict the emergence of body-centered-cubic order during annealing, with a clear crossover from disordered aggregation to crystallization as the attractions strengthen. Slower annealing and higher concentration both promote larger, more ordered crystallites, whereas an excessive graft length frustrates long-range order. Simulated cold sintering further reveals how compression merges crystalline grains into continuous networks while introducing structural defects. By directly linking NCT chemistry to assembly kinetics and final microstructure, this framework provides mechanistic insights and quantitative guidance for engineering nanoparticle superlattices with tailored order and connectivity.<\/jats:p>","DOI":"10.1021\/acsnano.6c09339","type":"journal-article","created":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T17:02:30Z","timestamp":1786986150000},"page":"24902-24914","source":"Crossref","is-referenced-by-count":0,"title":["Multiscale Design\nof Interaction-Driven Superlattice\nAssembly in Nanocomposite Tectons"],"prefix":"10.1021","volume":"20","author":[{"given":"Anushka","family":"Jha","sequence":"first","affiliation":[{"name":"Northeastern University , , , ,","place":["Boston, Massachusetts, United States, 02115"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-7084-4060","authenticated-orcid":true,"given":"Stephen","family":"Kronenberger","sequence":"additional","affiliation":[{"name":"University of Delaware , , , ,","place":["Newark, Delaware, United States, 19716"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5074-293X","authenticated-orcid":true,"given":"Carl","family":"Thrasher","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9945-3955","authenticated-orcid":true,"given":"Nicholas","family":"Sbalbi","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , , ,","place":["Cambridge, Massachusetts, United States, 02139"]},{"name":"Massachusetts Institute of Technology , , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6533-5897","authenticated-orcid":true,"given":"Matthew D.","family":"Ye","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9449-2680","authenticated-orcid":true,"given":"Robert","family":"Macfarlane","sequence":"additional","affiliation":[{"name":"Massachusetts Institute of Technology , , , ,","place":["Cambridge, Massachusetts, United States, 02139"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5295-4581","authenticated-orcid":true,"given":"Arthi","family":"Jayaraman","sequence":"additional","affiliation":[{"name":"University of Delaware , , , ,","place":["Newark, Delaware, United States, 19716"]},{"name":"University of Delaware , , , ,","place":["Newark, Delaware, United States, 19716"]},{"name":"University of Delaware , , , ,","place":["Newark, Delaware, United States, 19716"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-6031-3779","authenticated-orcid":true,"given":"Safa","family":"Jamali","sequence":"additional","affiliation":[{"name":"Northeastern University , , , ,","place":["Boston, Massachusetts, United States, 02115"]},{"name":"Northeastern University , , , ,","place":["Boston, Massachusetts, United States, 02115"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,17]]},"reference":[{"key":"2026091510114874700_cit1","doi-asserted-by":"publisher","first-page":"16228","DOI":"10.1021\/jacs.6b11052","article-title":"Self-assembling nanocomposite tectons","volume":"138","author":"Zhang","year":"2016","journal-title":"J. Am. Chem. Soc."},{"key":"2026091510114874700_cit2","doi-asserted-by":"publisher","first-page":"6391","DOI":"10.1021\/acs.analchem.9b00707","article-title":"Characterizing Polymer-Grafted Nanoparticles:\nFrom Basic Defining Parameters to Behavior in Solvents and Self-Assembled\nStructures","volume":"91","author":"Chancellor","year":"2019","journal-title":"Anal. Chem."},{"key":"2026091510114874700_cit3","first-page":"227","volume-title":"Spherical Nucleic\nAcids","author":"Laramy","year":"2020"},{"key":"2026091510114874700_cit4","doi-asserted-by":"publisher","first-page":"586","DOI":"10.1038\/s41586-021-03355-z","article-title":"Macroscopic\nmaterials assembled from nanoparticle superlattices","volume":"591","author":"Santos","year":"2021","journal-title":"Nature"},{"key":"2026091510114874700_cit5","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202107875","article-title":"Programmable\nmatter: the nanoparticle atom and DNA bond","volume":"34","author":"Samanta","year":"2022","journal-title":"Adv. Mater."},{"key":"2026091510114874700_cit6","doi-asserted-by":"publisher","first-page":"1248","DOI":"10.1021\/accountsmr.2c00153","article-title":"Hierarchically\nstructured nanocomposites via a \u201csystems materials science\u201d\napproach","volume":"3","author":"Li","year":"2022","journal-title":"Acc. Mater. Res."},{"key":"2026091510114874700_cit7","doi-asserted-by":"publisher","first-page":"20753","DOI":"10.1021\/acsnano.5c02810","article-title":"Forging Nanoparticle Superlattices\nwith Colloidal Metallurgy","volume":"19","author":"Thrasher","year":"2025","journal-title":"ACS Nano"},{"key":"2026091510114874700_cit8","doi-asserted-by":"publisher","first-page":"1342","DOI":"10.1039\/C8CS00787J","article-title":"Stimuli-responsive self-assembly\nof nanoparticles","volume":"48","author":"Grzelczak","year":"2019","journal-title":"Chem. Soc. Rev."},{"key":"2026091510114874700_cit9","doi-asserted-by":"publisher","first-page":"25248","DOI":"10.1021\/acsami.2c05378","article-title":"Nanoparticle Self-Assembly: From\nDesign Principles to Complex Matter to Functional Materials","volume":"15","author":"Rao","year":"2023","journal-title":"ACS Appl. Mater. Interfaces"},{"key":"2026091510114874700_cit10","doi-asserted-by":"publisher","first-page":"12351","DOI":"10.1021\/acs.nanolett.5c03009","article-title":"Acoustoplasmonic Metasurfaces\nBased on Polymer-Grafted Nanoparticles","volume":"25","author":"Vasileiadis","year":"2025","journal-title":"Nano\nLett."},{"key":"2026091510114874700_cit11","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202410493","article-title":"Regio-Selective\nMechanical Enhancement of Polymer-Grafted Nanoparticle Composites\nvia Light-Mediated Crosslinking","volume":"37","author":"Kim","year":"2025","journal-title":"Adv. Mater."},{"key":"2026091510114874700_cit12","doi-asserted-by":"publisher","first-page":"14791","DOI":"10.1021\/acsnano.3c10201","article-title":"Nanocrystal\nassemblies: Current advances and open problems","volume":"18","author":"Bassani","year":"2024","journal-title":"ACS Nano"},{"key":"2026091510114874700_cit13","doi-asserted-by":"publisher","DOI":"10.1038\/natrevmats.2015.11","article-title":"Assembly and phase transitions of\ncolloidal crystals","volume":"1","author":"Li","year":"2016","journal-title":"Nat. Rev. Mater."},{"key":"2026091510114874700_cit14","doi-asserted-by":"publisher","first-page":"1102","DOI":"10.3390\/mi13071102","article-title":"Self-assembly\nof DNA-grafted colloids: a review of challenges","volume":"13","author":"Dwivedi","year":"2022","journal-title":"Micromachines"},{"key":"2026091510114874700_cit15","doi-asserted-by":"publisher","first-page":"1020","DOI":"10.1038\/35059035","article-title":"Prediction of absolute\ncrystal-nucleation rate in hard-sphere\ncolloids","volume":"409","author":"Auer","year":"2001","journal-title":"Nature"},{"key":"2026091510114874700_cit16","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.123.258002","article-title":"Influence of hydrodynamic\ninteractions on colloidal crystallization","volume":"123","author":"Tateno","year":"2019","journal-title":"Phys.\nRev. Lett."},{"key":"2026091510114874700_cit17","doi-asserted-by":"publisher","first-page":"1847","DOI":"10.1039\/D5SM01128K","article-title":"Molecular dynamics simulation of self-assembly of one-component\nnanocrystals grafted with end-functionalized polymers","volume":"22","author":"Deng","year":"2026","journal-title":"Soft Matter"},{"key":"2026091510114874700_cit18","doi-asserted-by":"publisher","first-page":"1445","DOI":"10.1051\/jphys:0197600370120144500","article-title":"Scaling theory of polymer adsorption","volume":"37","author":"De Gennes","year":"1976","journal-title":"J. Phys."},{"key":"2026091510114874700_cit19","doi-asserted-by":"publisher","first-page":"983","DOI":"10.1051\/jphys:01977003808098300","article-title":"Adsorption\nof chain molecules with a polar head a scaling description","volume":"38","author":"Alexander","year":"1977","journal-title":"J. Phys."},{"key":"2026091510114874700_cit20","doi-asserted-by":"publisher","first-page":"1600","DOI":"10.1002\/smll.200900358","article-title":"Nanoscale\nforces and their uses in self-assembly","volume":"5","author":"Bishop","year":"2009","journal-title":"Small"},{"key":"2026091510114874700_cit21","doi-asserted-by":"publisher","first-page":"14624","DOI":"10.1021\/jacs.9b04999","article-title":"Dictating\nnanoparticle assembly via systems-level control of molecular multivalency","volume":"141","author":"Santos","year":"2019","journal-title":"J. Am. Chem. Soc."},{"key":"2026091510114874700_cit22","doi-asserted-by":"publisher","first-page":"751","DOI":"10.1080\/08927022.2012.683528","article-title":"Integrating PRISM theory and Monte Carlo simulation to study polymer-functionalised\nparticles and polymer nanocomposites","volume":"38","author":"Jayaraman","year":"2012","journal-title":"Mol. Simul."},{"key":"2026091510114874700_cit23","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevLett.110.018301","article-title":"Polydispersity\nfor Tuning the Potential\nof Mean Force between Polymer Grafted Nanoparticles in a Polymer Matrix","volume":"110","author":"Martin","year":"2013","journal-title":"Phys. Rev. Lett."},{"key":"2026091510114874700_cit24","doi-asserted-by":"publisher","first-page":"13","DOI":"10.1039\/C3SM51864G","article-title":"Theory and\nsimulation studies of effective interactions,\nphase behavior and morphology in polymer nanocomposites","volume":"10","author":"Ganesan","year":"2014","journal-title":"Soft Matter"},{"key":"2026091510114874700_cit25","doi-asserted-by":"publisher","DOI":"10.1073\/pnas.2316394121","article-title":"Network physics\nof attractive colloidal gels: Resilience, rigidity, and phase diagram","volume":"121","author":"Nabizadeh","year":"2024","journal-title":"Proc. Natl. Acad. Sci. U.S.A."},{"key":"2026091510114874700_cit26","doi-asserted-by":"publisher","first-page":"7904","DOI":"10.1039\/D5SM00572H","article-title":"Emergence and evolution of a particulate\nnetwork during gelation and coarsening of attractive colloids","volume":"21","author":"Haghighi","year":"2025","journal-title":"Soft Matter"},{"key":"2026091510114874700_cit27","doi-asserted-by":"publisher","first-page":"5774","DOI":"10.1021\/acs.nanolett.9b02508","article-title":"Assembling ordered crystals with\ndisperse building blocks","volume":"19","author":"Santos","year":"2019","journal-title":"Nano Lett."},{"key":"2026091510114874700_cit28","doi-asserted-by":"publisher","first-page":"4466","DOI":"10.1039\/D4SM00209A","article-title":"Role of interaction\nrange on the microstructure and\ndynamics of attractive colloidal systems","volume":"20","author":"Mangal","year":"2024","journal-title":"Soft\nMatter"},{"key":"2026091510114874700_cit29","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-025-58959-0","article-title":"Direct observation\nand control of\nnon-classical crystallization pathways in binary colloidal systems","volume":"16","author":"Zang","year":"2025","journal-title":"Nat. Commun."},{"key":"2026091510114874700_cit30","doi-asserted-by":"publisher","first-page":"1170","DOI":"10.1021\/jacs.9b11476","article-title":"Reinforcing\nsupramolecular bonding with magnetic dipole\ninteractions to assemble dynamic nanoparticle superlattices","volume":"142","author":"Santos","year":"2020","journal-title":"J. Am. Chem. Soc."},{"key":"2026091510114874700_cit31","doi-asserted-by":"publisher","DOI":"10.1103\/PhysRevB.73.054104","article-title":"Applications of local crystal structure measures in\nexperiment and simulation","volume":"73","author":"Ackland","year":"2006","journal-title":"Phys. Rev. B"},{"key":"2026091510114874700_cit32","doi-asserted-by":"publisher","first-page":"15970","DOI":"10.1021\/acsnano.4c04192","article-title":"Nanoparticle\nSuperlattices with Nonequilibrium Crystal\nShapes","volume":"18","author":"Ye","year":"2024","journal-title":"ACS Nano"},{"key":"2026091510114874700_cit33","doi-asserted-by":"publisher","first-page":"305","DOI":"10.1021\/la9808418","article-title":"Pore size distributions\nin porous glasses: a computer\nsimulation study","volume":"15","author":"Gelb","year":"1999","journal-title":"Langmuir"},{"key":"2026091510114874700_cit34","volume-title":"Polymer Physics","author":"Rubinstein","year":"2020"},{"key":"2026091510114874700_cit35","doi-asserted-by":"publisher","DOI":"10.1016\/j.cpc.2021.108171","article-title":"LAMMPS-a\nflexible simulation tool for particle-based materials modeling at\nthe atomic, meso, and continuum scales","volume":"271","author":"Thompson","year":"2022","journal-title":"Comput.\nPhys. Commun."},{"key":"2026091510114874700_cit36","unstructured":"Grossfield, A.\n          \n          WHAM:\nThe Weighted Histogram Analysis Method. http:\/\/membrane.urmc.rochester.edu\/wordpress\/?page_id\/126."},{"key":"2026091510114874700_cit37","doi-asserted-by":"publisher","DOI":"10.1016\/j.commatsci.2019.109363","article-title":"HOOMD-blue:\nA Python package for\nhigh-performance molecular dynamics and hard particle Monte Carlo\nsimulations","volume":"173","author":"Anderson","year":"2020","journal-title":"Comput. Mater. Sci."},{"key":"2026091510114874700_cit38","doi-asserted-by":"publisher","DOI":"10.1063\/1.2977970","article-title":"Accurate determination\nof crystal structures based\non averaged local bond order parameters","volume":"129","author":"Lechner","year":"2008","journal-title":"J.\nChem. Phys."}],"container-title":["ACS Nano"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/pubs.acs.org\/doi\/pdf\/10.1021\/acsnano.6c09339","content-type":"application\/pdf","content-version":"vor","intended-application":"unspecified"},{"URL":"https:\/\/pubs.acs.org\/ancac3\/article-pdf\/20\/36\/24902\/66652226\/acsnano.6c09339.pdf","content-type":"application\/pdf","content-version":"vor","intended-application":"syndication"},{"URL":"https:\/\/pubs.acs.org\/ancac3\/article-pdf\/20\/36\/24902\/66652226\/acsnano.6c09339.pdf","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2026,9,15]],"date-time":"2026-09-15T14:51:15Z","timestamp":1789483875000},"score":1,"resource":{"primary":{"URL":"https:\/\/pubs.acs.org\/ancac3\/article\/20\/36\/24902\/5262327\/Multiscale-Design-of-Interaction-Driven"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2026,8,17]]},"references-count":38,"journal-issue":{"issue":"36","published-online":{"date-parts":[[2026,8,17]]},"published-print":{"date-parts":[[2026,9,15]]}},"URL":"https:\/\/doi.org\/10.1021\/acsnano.6c09339","relation":{},"ISSN":["1936-0851","1936-086X"],"issn-type":[{"value":"1936-0851","type":"print"},{"value":"1936-086X","type":"electronic"}],"subject":[],"published":{"date-parts":[[2026,8,17]]}}}