Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals

Igor Coropceanu^#¹, Eric M Janke^#¹, Joshua Portner^#¹, Danny Haubold^{1

2}, Trung Dac Nguyen³, Avishek Das⁴, Christian P N Tanner⁴, James K Utterback⁴, Samuel W Teitelbaum⁵, Margaret H Hudson¹, Nivedina A Sarma¹, Alex M Hinkle¹, Christopher J Tassone⁶, Alexander Eychmüller², David T Limmer^{4

7

8}, Monica Olvera de la Cruz^{3

9}, Naomi S Ginsberg^{4

8

10

11}, Dmitri V Talapin^{1

12}

Affiliations

¹ Department of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL 60637, USA.
² Physical Chemistry, Technische Universität Dresden, Dresden, Germany.
³ Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL 60208, USA.
⁴ Department of Chemistry, University of California, Berkeley, CA 94720, USA.
⁵ Department of Physics and Beus CXFEL Labs, Biodesign Institute, Arizona State University, Tempe, AZ 85287, USA.
⁶ Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
⁷ Chemical Sciences Division and Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
⁸ Kavli Energy NanoSciences Institute, University of California, Berkeley, CA 94720, USA.
⁹ Department of Materials Science and Engineering, Department of Chemistry, and Department of Physics and Astronomy, Northwestern University, Evanston, IL 60208, USA.
¹⁰ Department of Physics, University of California, Berkeley, CA 94720, USA.
¹¹ Materials Sciences Division, Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
¹² Center for Nanoscale Materials, Argonne National Laboratory, Argonne, IL 60517, USA.

^# Contributed equally.

PMID: 35324292
DOI: 10.1126/science.abm6753

Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals

Igor Coropceanu et al. Science. 2022.

. 2022 Mar 25;375(6587):1422-1426.

doi: 10.1126/science.abm6753. Epub 2022 Mar 24.

Authors

Affiliations

¹ Department of Chemistry, James Franck Institute, and Pritzker School of Molecular Engineering, University of Chicago, Chicago, IL 60637, USA.
² Physical Chemistry, Technische Universität Dresden, Dresden, Germany.
³ Department of Chemical and Biological Engineering, Northwestern University, Evanston, IL 60208, USA.
⁴ Department of Chemistry, University of California, Berkeley, CA 94720, USA.
⁵ Department of Physics and Beus CXFEL Labs, Biodesign Institute, Arizona State University, Tempe, AZ 85287, USA.
⁶ Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, Menlo Park, CA 94025, USA.
⁷ Chemical Sciences Division and Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
⁸ Kavli Energy NanoSciences Institute, University of California, Berkeley, CA 94720, USA.
⁹ Department of Materials Science and Engineering, Department of Chemistry, and Department of Physics and Astronomy, Northwestern University, Evanston, IL 60208, USA.
¹⁰ Department of Physics, University of California, Berkeley, CA 94720, USA.
¹¹ Materials Sciences Division, Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA.
¹² Center for Nanoscale Materials, Argonne National Laboratory, Argonne, IL 60517, USA.

^# Contributed equally.

PMID: 35324292
DOI: 10.1126/science.abm6753

Abstract

Colloidal nanocrystals of metals, semiconductors, and other functional materials can self-assemble into long-range ordered crystalline and quasicrystalline phases, but insulating organic surface ligands prevent the development of collective electronic states in ordered nanocrystal assemblies. We reversibly self-assembled colloidal nanocrystals of gold, platinum, nickel, lead sulfide, and lead selenide with conductive inorganic ligands into supercrystals exhibiting optical and electronic properties consistent with strong electronic coupling between the constituent nanocrystals. The phase behavior of charge-stabilized nanocrystals can be rationalized and navigated with phase diagrams computed for particles interacting through short-range attractive potentials. By finely tuning interparticle interactions, the assembly was directed either through one-step nucleation or nonclassical two-step nucleation pathways. In the latter case, the nucleation was preceded by the formation of two metastable colloidal fluids.

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Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals

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Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals

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Abstract

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