Christian P. N. Tanner, Vivian R. K. Wall, Joshua Portner, Ahhyun Jeong, Avishek Das, James K. Utterback, Leo M. Hamerlynck, Jonathan G. Raybin, Matthew J. Hurley, Nicholas Leonard, Rebecca B. Wai, Jenna A. Tan, Mumtaz Gababa, Chenhui Zhu, Eric Schaible, Christopher J. Tassone, David T. Limmer, Samuel W. Teitelbaum, Dmitri V. Talapin, Naomi S. Ginsberg
{"title":"在亚稳液体双节点附近增强纳米级带电胶体结晶","authors":"Christian P. N. Tanner, Vivian R. K. Wall, Joshua Portner, Ahhyun Jeong, Avishek Das, James K. Utterback, Leo M. Hamerlynck, Jonathan G. Raybin, Matthew J. Hurley, Nicholas Leonard, Rebecca B. Wai, Jenna A. Tan, Mumtaz Gababa, Chenhui Zhu, Eric Schaible, Christopher J. Tassone, David T. Limmer, Samuel W. Teitelbaum, Dmitri V. Talapin, Naomi S. Ginsberg","doi":"10.1038/s41567-025-02996-5","DOIUrl":null,"url":null,"abstract":"<p>Achieving predictive control over crystallization using non-classical nucleation while avoiding kinetic traps would be a step towards designing materials with new functionalities. We address these challenges by inducing the bottom-up assembly of nanocrystals into ordered arrays, or superlattices. Using electrostatics—rather than density—to tune the interactions between particles, we watch self-assembly proceed through a metastable liquid phase. We systematically investigate the phase behaviour as a function of quench conditions in situ and in real time using small-angle X-ray scattering. By fitting to colloid, liquid and superlattice models, we extract the time evolution of each phase and the system phase diagram, which we find to be consistent with short-range attractive interactions. Using the predictive power of the phase diagram, we establish control of the self-assembly rate over three orders of magnitude, and we identify one- and two-step self-assembly regimes, with only the latter implicating the metastable liquid as an intermediate. The presence of the metastable liquid increases the superlattice formation rate relative to the equivalent one-step pathway, and the superlattice order increases with the rate, revealing a generalizable kinetic strategy for promoting and enhancing ordered assembly.</p>","PeriodicalId":19100,"journal":{"name":"Nature Physics","volume":"185 1","pages":""},"PeriodicalIF":18.4000,"publicationDate":"2025-08-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancing nanoscale charged colloid crystallization near a metastable liquid binodal\",\"authors\":\"Christian P. N. Tanner, Vivian R. K. Wall, Joshua Portner, Ahhyun Jeong, Avishek Das, James K. Utterback, Leo M. Hamerlynck, Jonathan G. Raybin, Matthew J. Hurley, Nicholas Leonard, Rebecca B. Wai, Jenna A. Tan, Mumtaz Gababa, Chenhui Zhu, Eric Schaible, Christopher J. Tassone, David T. Limmer, Samuel W. Teitelbaum, Dmitri V. Talapin, Naomi S. Ginsberg\",\"doi\":\"10.1038/s41567-025-02996-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Achieving predictive control over crystallization using non-classical nucleation while avoiding kinetic traps would be a step towards designing materials with new functionalities. We address these challenges by inducing the bottom-up assembly of nanocrystals into ordered arrays, or superlattices. Using electrostatics—rather than density—to tune the interactions between particles, we watch self-assembly proceed through a metastable liquid phase. We systematically investigate the phase behaviour as a function of quench conditions in situ and in real time using small-angle X-ray scattering. By fitting to colloid, liquid and superlattice models, we extract the time evolution of each phase and the system phase diagram, which we find to be consistent with short-range attractive interactions. Using the predictive power of the phase diagram, we establish control of the self-assembly rate over three orders of magnitude, and we identify one- and two-step self-assembly regimes, with only the latter implicating the metastable liquid as an intermediate. The presence of the metastable liquid increases the superlattice formation rate relative to the equivalent one-step pathway, and the superlattice order increases with the rate, revealing a generalizable kinetic strategy for promoting and enhancing ordered assembly.</p>\",\"PeriodicalId\":19100,\"journal\":{\"name\":\"Nature Physics\",\"volume\":\"185 1\",\"pages\":\"\"},\"PeriodicalIF\":18.4000,\"publicationDate\":\"2025-08-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Nature Physics\",\"FirstCategoryId\":\"101\",\"ListUrlMain\":\"https://doi.org/10.1038/s41567-025-02996-5\",\"RegionNum\":1,\"RegionCategory\":\"物理与天体物理\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"PHYSICS, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Nature Physics","FirstCategoryId":"101","ListUrlMain":"https://doi.org/10.1038/s41567-025-02996-5","RegionNum":1,"RegionCategory":"物理与天体物理","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"PHYSICS, MULTIDISCIPLINARY","Score":null,"Total":0}
Enhancing nanoscale charged colloid crystallization near a metastable liquid binodal
Achieving predictive control over crystallization using non-classical nucleation while avoiding kinetic traps would be a step towards designing materials with new functionalities. We address these challenges by inducing the bottom-up assembly of nanocrystals into ordered arrays, or superlattices. Using electrostatics—rather than density—to tune the interactions between particles, we watch self-assembly proceed through a metastable liquid phase. We systematically investigate the phase behaviour as a function of quench conditions in situ and in real time using small-angle X-ray scattering. By fitting to colloid, liquid and superlattice models, we extract the time evolution of each phase and the system phase diagram, which we find to be consistent with short-range attractive interactions. Using the predictive power of the phase diagram, we establish control of the self-assembly rate over three orders of magnitude, and we identify one- and two-step self-assembly regimes, with only the latter implicating the metastable liquid as an intermediate. The presence of the metastable liquid increases the superlattice formation rate relative to the equivalent one-step pathway, and the superlattice order increases with the rate, revealing a generalizable kinetic strategy for promoting and enhancing ordered assembly.
期刊介绍:
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