Enhancing nanocrystal superlattice self-assembly near a metastable liquid binodal

ORAL

Abstract

Self-assembly of colloidal nanocrystals (NCs) into superlattices (SLs) is an appealing strategy to design hierarchically organized materials with new functionalities. Mechanistic studies are needed to uncover SL self-assembly design principles, but they are difficult to perform due to the fast time- and short length scales of NC systems. To address this challenge, we developed an apparatus to directly measure in situ and in real time solutions of electrostatically stabilized NCs as they are quenched to form SLs using small angle X-ray scattering. By developing a quantitative model, we fit the time-dependent scattering patterns to obtain the phase diagram of the system and the kinetics as a function of varying quench conditions. The extracted phase diagram is consistent with particles whose interactions are short in range relative to their size. As a result, we can direct the self-assembly through one-step or two-step pathways in which SLs form either directly from the colloidal phase or from a metastable liquid intermediate whose fluctuations we quantified using X-ray photon correlation spectroscopy. By combining this in situ methodology with quantitative analysis tools and simulation, we propose design principles and kinetic strategies to optimize nanoscale self-assembly.

*This work was supported by the US Department of Energy under award no. DE-SC0019375 and by the National Science Foundation Graduate Research Fellowship.

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Publication: Christian P. N. Tanner, Vivian Wall, Mumtaz Gababa, Joshua Portner, James K. Utterback, Leo Hamerlynck, Jonathan Raybin, Matthew Hurley, Ahhyun Jeong, Ahyoung Kim, Andrei Fluerasu, Yanwen Sun, David Limmer, Samuel Teitelbaum, Dmitri Talapin, Naomi S. Ginsberg. "Nanoscopic fluctuations of electrostatically stabilized colloidal and condensed semiconductor nanocrystals elucidated by MHz X-ray photon correlation spectroscopy," In preparation (2023).
Christian P. N. Tanner*, Vivian Wall*, Joshua Portner, James K. Utterback, Leo Hamerlynck, Jonathan Raybin, Matthew Hurley, Ahhyun Jeong, Mumtaz Gababa, Rebecca Wai, Jenna Tan, Avishek Das, Igor Coropceanu, Eric M. Janke, Christopher Tassone, Chenhui Zhu, David Limmer, Samuel Teitelbaum, Dmitri Talapin, Naomi S. Ginsberg. "Quench-dependent kinetics of strongly coupled lead sulfide nanocrystal superlattice self-assembly in electrolytic environments unveiled via in situ X-ray scattering," In preparation (2023).
Matthew Hurley*, Christian P. N. Tanner*, Joshua Portner, James K. Utterback, Igor Coropceanu, Avishek Das, Yanwen Sun, Garth Williams, Sanghoon Song, David Limmer, Dmitri Talapin, Naomi S. Ginsberg, Samuel Teitelbaum. "In situ coherent X-ray scattering reveals polycrystalline structure and discrete annealing events in strongly coupled nanocrystal superlattices," In preparation (2023).
Christian P. N. Tanner, James K. Utterback, Igor Coropceanu, Joshua Portner, Avishek Das, Vivian Wall, Eric M. Janke, Christopher Tassone, David Limmer, Samuel Teitelbaum, Dmitri Talapin, Naomi S. Ginsberg. "Phase evolution of electrostatically stabilized metal nanocrystals unveiled via in situ X-ray scattering," In preparation (2023).
I. Coropceanu, E. M. Janke, J. Portner, D. Haubold, T. D. Nguyen, A. Das, C. P. N. Tanner, J. K. Utterback, S. W. Teitelbaum, M. H. Hudson, N. A. Sarma, A. M. Hinkle, C. J. Tassone, A. Eychmüller, D. T. Limmer, M. Olvera de La Cruz, N. S. Ginsberg, D. V. Talapin, "Self-assembly of nanocrystals into strongly electronically coupled all-inorganic supercrystals," Science, 375,

Presenters

  • Christian Tanner

    • University of California Berkeley

Authors

  • Christian Tanner

    • University of California Berkeley

  • Vivian R Wall

    • UC Berkeley

  • Josh Portner

    • University of Chicago

  • Avishek Das

    • University of California, Berkeley

  • James Utterback

    • University of California Berkeley

  • Ahhyun Jeong

    • University of Chicago

  • Mumtaz Gababa

    • University of California Berkeley

  • Igor Coropceanu

    • University of Chicago

  • Leo Hamerlynck

    • University of California Berkeley

  • Jonathan Raybin

    • University of California Berkeley

  • Matthew Hurley

    • Arizona State University

  • Nicholas Leonard

    • Arizona State University

  • Ahyoung Kim

    • University of Illinois Urbana-Champaign
    • University of California Berkeley

  • Christopher J Tassone

    • SLAC National Accelerator Laboratory

  • Andrei Fluerasu

    • Brookhaven National Laboratory
    • NSLS2, Brookhaven National Lab

  • Yanwen Sun

    • SLAC NATIONAL ACCELERATOR LABORATORY
    • SLAC National Accelerator Laboratory

  • David T Limmer

    • University of California, Berkeley

  • Samuel W Teitelbaum

    • Arizona State University

  • Dmitri V Talapin

    • University of Chicago

  • Naomi S Ginsberg

    • University of California, Berkeley