Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films

Michela Sainato, Brian Shevitski, Ayaskanta Sahu, Jason D. Forster, Shaul Aloni, Giuseppe Barillaro, Jeffrey J. Urban

Research output: Contribution to journalArticle

Abstract

Self-assembly of semiconductor nanocrystals (NCs) into two-dimensional patterns or three-dimensional (2-3D) superstructures has emerged as a promising low-cost route to generate thin-film transistors and solar cells with superior charge transport because of enhanced electronic coupling between the NCs. Here, we show that lead sulfide (PbS) NCs solids featuring either short-range (disordered glassy solids, GSs) or long-range (superlattices, SLs) packing order are obtained solely by controlling deposition conditions of colloidal solution of NCs. In this study, we demonstrate the use of the evaporation-driven self-assembly method results in PbS NC SL structures that are observed over an area of 1 mm × 100 μm, with long-range translational order of up to 100 nm. A number of ordered domains appear to have nucleated simultaneously and grown together over the whole area, imparting a polycrystalline texture to the 3D SL films. By contrast, a conventional, optimized spin-coating deposition method results in PbS NC glassy films with no translational symmetry and much shorter-range packing order in agreement with state-of-the-art reports. Further, we investigate the electronic properties of both SL and GS films, using a field-effect transistor configuration as a test platform. The long-range ordering of the PbS NCs into SLs leads to semiconducting NC-based solids, the mobility (μ) of which is 3 orders of magnitude higher than that of the disordered GSs. Moreover, although spin-cast GSs of PbS NCs have weak ambipolar behavior with limited gate tunability, SLs of PbS NCs show a clear p-type behavior with significantly higher conductivities.

Original languageEnglish (US)
Pages (from-to)3381-3690
Number of pages310
JournalACS Omega
Volume2
Issue number7
DOIs
StatePublished - Jul 31 2017

Fingerprint

Nanocrystals
Charge transfer
Self assembly
Superlattices
Crystal symmetry
Spin coating
Thin film transistors
Field effect transistors
Electronic properties
Solar cells
Evaporation
Textures
Lead
Semiconductor materials

ASJC Scopus subject areas

  • Chemical Engineering(all)
  • Chemistry(all)

Cite this

Sainato, M., Shevitski, B., Sahu, A., Forster, J. D., Aloni, S., Barillaro, G., & Urban, J. J. (2017). Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films. ACS Omega, 2(7), 3381-3690. https://doi.org/10.1021/acsomega.7b00433

Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films. / Sainato, Michela; Shevitski, Brian; Sahu, Ayaskanta; Forster, Jason D.; Aloni, Shaul; Barillaro, Giuseppe; Urban, Jeffrey J.

In: ACS Omega, Vol. 2, No. 7, 31.07.2017, p. 3381-3690.

Research output: Contribution to journalArticle

Sainato, M, Shevitski, B, Sahu, A, Forster, JD, Aloni, S, Barillaro, G & Urban, JJ 2017, 'Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films', ACS Omega, vol. 2, no. 7, pp. 3381-3690. https://doi.org/10.1021/acsomega.7b00433
Sainato M, Shevitski B, Sahu A, Forster JD, Aloni S, Barillaro G et al. Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films. ACS Omega. 2017 Jul 31;2(7):3381-3690. https://doi.org/10.1021/acsomega.7b00433
Sainato, Michela ; Shevitski, Brian ; Sahu, Ayaskanta ; Forster, Jason D. ; Aloni, Shaul ; Barillaro, Giuseppe ; Urban, Jeffrey J. / Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films. In: ACS Omega. 2017 ; Vol. 2, No. 7. pp. 3381-3690.
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