Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films
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,more »
- Authors:
-
- Dipartimento di Ingegneria dell’Informazione, Università di Pisa, Via G. Caruso 16, 56111 Pisa, Italy
- Molecular Foundry, Lawrence Berkeley National Laboratory, 67 Cyclotron Road, 94720 Berkeley, United States
- Publication Date:
- Research Org.:
- Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). Molecular Foundry
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1371598
- Alternate Identifier(s):
- OSTI ID: 1376694; OSTI ID: 1630601
- Grant/Contract Number:
- AC02-05CH11231
- Resource Type:
- Published Article
- Journal Name:
- ACS Omega
- Additional Journal Information:
- Journal Name: ACS Omega Journal Volume: 2 Journal Issue: 7; Journal ID: ISSN 2470-1343
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; crystal structure; electric transport processes and properties; microstructure; nanocrystals; order; phase; quantum dots; self-assembly; solid state electrochemistry; thin films; solid state
Citation Formats
Sainato, Michela, Shevitski, Brian, Sahu, Ayaskanta, Forster, Jason D., Aloni, Shaul, Barillaro, Giuseppe, and Urban, Jeffrey J. Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films. United States: N. p., 2017.
Web. doi: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. United States. https://doi.org/10.1021/acsomega.7b00433
Sainato, Michela, Shevitski, Brian, Sahu, Ayaskanta, Forster, Jason D., Aloni, Shaul, Barillaro, Giuseppe, and Urban, Jeffrey J. Tue .
"Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films". United States. https://doi.org/10.1021/acsomega.7b00433.
@article{osti_1371598,
title = {Long-Range Order in Nanocrystal Assemblies Determines Charge Transport of Films},
author = {Sainato, Michela and Shevitski, Brian and Sahu, Ayaskanta and Forster, Jason D. and Aloni, Shaul and Barillaro, Giuseppe and Urban, Jeffrey J.},
abstractNote = {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.},
doi = {10.1021/acsomega.7b00433},
journal = {ACS Omega},
number = 7,
volume = 2,
place = {United States},
year = {Tue Jul 18 00:00:00 EDT 2017},
month = {Tue Jul 18 00:00:00 EDT 2017}
}
https://doi.org/10.1021/acsomega.7b00433
Web of Science
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