Colloidal Atomic Layer Deposition with Stationary Reactant Phases Enables Precise Synthesis of “Digital” II–VI Nano-heterostructures with Exquisite Control of Confinement and Strain

Hazarika, Abhijit; Fedin, Igor; Hong, Liang; Guo, Jinglong; Srivastava, Vishwas; Cho, Wooje; Coropceanu, Igor; Portner, Joshua; Diroll, Benjamin T.; Philbin, John P.; Rabani, Eran; Klie, Robert; Talapin, Dmitri V.

doi:10.1021/jacs.9b04866

Title: Colloidal Atomic Layer Deposition with Stationary Reactant Phases Enables Precise Synthesis of “Digital” II–VI Nano-heterostructures with Exquisite Control of Confinement and Strain

Journal Article · Sat Aug 03 00:00:00 EDT 2019 · Journal of the American Chemical Society

DOI:https://doi.org/10.1021/jacs.9b04866· OSTI ID:1561241

^[1]; Fedin, Igor ^[1];

^[1]; Guo, Jinglong ^[1]; Srivastava, Vishwas ^[1];

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^[1]; Portner, Joshua ^[1];

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^[3];

^[4]; Klie, Robert ^[1];

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Univ. of Chicago, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Tel Aviv Univ., Ramat Aviv (Israel)
Univ. of Chicago, IL (United States); Argonne National Lab. (ANL), Lemont, IL (United States)

In contrast to molecular systems, which are defined with atomic precision, nanomaterials generally show some heterogeneity in size, shape, and composition. The sample inhomogeneity translates into a distribution of energy levels, band gaps, work functions, and other characteristics, which detrimentally affect practically every property of functional nanomaterials. Here, we introduce a novel synthetic strategy, colloidal atomic layer deposition (c-ALD) with stationary reactant phases, which largely circumvents the limitations of traditional colloidal syntheses of nano-heterostructures with atomic precision. This method allows for significant reduction of inhomogeneity in nanomaterials in complex nanostructures without compromising their structural perfection and enables the synthesis of epitaxial nano-heterostructures of unprecedented complexity. The improved synthetic control ultimately enables bandgap and strain engineering in colloidal nanomaterials with close to atomic accuracy. To demonstrate the power of the new c-ALD method, we synthesize a library of complex II–VI semiconductor nanoplatelet heterostructures. By combining spectroscopic and computational studies, we elucidate the subtle interplay between quantum confinement and strain effects on the optical properties of semiconductor nanostructures.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); US Air Force Office of Scientific Research (AFOSR)