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.
Coropceanu, Igor, Janke, Eric M., Portner, Joshua, Haubold, Danny, Nguyen, Trung Dac, Das, Avishek, Tanner, Christian N., Utterback, James K., Teitelbaum, Samuel W., Hudson, ¸. H., Sarma, Nivedina A., Hinkle, Alex M., Tassone, Christopher J., Eychmüller, Alexander, Limmer, David T., Olvera de la Cruz, Monica, Ginsberg, Naomi S., & Talapin, Dmitri V. (2022). Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals. Science, 375(6587). https://doi.org/10.1126/science.abm6753
Coropceanu, Igor, Janke, Eric M., Portner, Joshua, et al., "Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals," Science 375, no. 6587 (2022), https://doi.org/10.1126/science.abm6753
@article{osti_1866599,
author = {Coropceanu, Igor and Janke, Eric M. and Portner, Joshua and Haubold, Danny and Nguyen, Trung Dac and Das, Avishek and Tanner, Christian N. and Utterback, James K. and Teitelbaum, Samuel W. and Hudson, ¸. H. and others},
title = {Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals},
annote = {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.},
doi = {10.1126/science.abm6753},
url = {https://www.osti.gov/biblio/1866599},
journal = {Science},
issn = {ISSN 0036-8075},
number = {6587},
volume = {375},
place = {United States},
publisher = {AAAS},
year = {2022},
month = {03}}
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); Deutsche Forschungsgemeinschaft; National Science Foundation (NSF); Alfred P. Sloan Research Fellowship; Packard Foundation