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Title: Modulation of Carrier Type in Nanocrystal-in-Matrix Composites by Interfacial Doping

Inorganic nanocomposites synthesized by combination of colloidal nanocrystals (NCs) and inorganic clusters have recently emerged as new materials with novel and unique functionalities. Much of the demonstrated promise of nanocomposites derives from the unique interactions between NC and matrix components—this generates new material properties, which direct unique transport behavior in the overall solid or nanocomposite—be it mass, charge, or heat. While measured empirically, it has remained largely impossible to take an a priori look at material properties and use those as a guideline to design desired transport behavior. Fundamentally, this is because the structural and electronic changes manifest at those interfaces have remained hidden from examination. We provide experimental evidence that transport behavior in nanocrystal-in-matrix (NIM) composites is dictated primarily by interfacial charge transfer associated with electronic and structural reconstructions as the composite forms. Our approach building continuous composite superlattices serves as a starting point for systematic probing of the nanointerface of NIM composites via ultrathin films. A combination of field effect transistor device characterization and photoemission spectroscopy reveals the systematic dependence of the polarity of charge transfer on the selection of matrix materials in NIM composites. We use this insight to combine, by design, different components to tune themore » carrier type in NIM composites.« less
Authors:
 [1] ;  [1] ;  [1] ; ORCiD logo [1] ;  [1] ; ORCiD logo [1] ;  [2] ;  [2] ;  [2] ; ORCiD logo [1] ;  [3] ;  [1] ; ORCiD logo [4]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). The Molecular Foundry; Univ. of Texas, Austin, TX (United States). McKetta Dept. of Chemical Engineering
Publication Date:
Grant/Contract Number:
AC02-76SF00515; F-1848; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Chemistry of Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 8; Journal ID: ISSN 0897-4756
Publisher:
American Chemical Society (ACS)
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Welch Foundation
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1470751

Sharma, Richa, Sawvel, April M., Barton, Bastian, Dong, Angang, Buonsanti, Raffaella, Llordes, Anna, Schaible, Eric, Axnanda, Stephanus, Liu, Zhi, Urban, Jeffrey J., Nordlund, Dennis, Kisielowski, Christian, and Milliron, Delia J.. Modulation of Carrier Type in Nanocrystal-in-Matrix Composites by Interfacial Doping. United States: N. p., Web. doi:10.1021/acs.chemmater.7b04689.
Sharma, Richa, Sawvel, April M., Barton, Bastian, Dong, Angang, Buonsanti, Raffaella, Llordes, Anna, Schaible, Eric, Axnanda, Stephanus, Liu, Zhi, Urban, Jeffrey J., Nordlund, Dennis, Kisielowski, Christian, & Milliron, Delia J.. Modulation of Carrier Type in Nanocrystal-in-Matrix Composites by Interfacial Doping. United States. doi:10.1021/acs.chemmater.7b04689.
Sharma, Richa, Sawvel, April M., Barton, Bastian, Dong, Angang, Buonsanti, Raffaella, Llordes, Anna, Schaible, Eric, Axnanda, Stephanus, Liu, Zhi, Urban, Jeffrey J., Nordlund, Dennis, Kisielowski, Christian, and Milliron, Delia J.. 2018. "Modulation of Carrier Type in Nanocrystal-in-Matrix Composites by Interfacial Doping". United States. doi:10.1021/acs.chemmater.7b04689. https://www.osti.gov/servlets/purl/1470751.
@article{osti_1470751,
title = {Modulation of Carrier Type in Nanocrystal-in-Matrix Composites by Interfacial Doping},
author = {Sharma, Richa and Sawvel, April M. and Barton, Bastian and Dong, Angang and Buonsanti, Raffaella and Llordes, Anna and Schaible, Eric and Axnanda, Stephanus and Liu, Zhi and Urban, Jeffrey J. and Nordlund, Dennis and Kisielowski, Christian and Milliron, Delia J.},
abstractNote = {Inorganic nanocomposites synthesized by combination of colloidal nanocrystals (NCs) and inorganic clusters have recently emerged as new materials with novel and unique functionalities. Much of the demonstrated promise of nanocomposites derives from the unique interactions between NC and matrix components—this generates new material properties, which direct unique transport behavior in the overall solid or nanocomposite—be it mass, charge, or heat. While measured empirically, it has remained largely impossible to take an a priori look at material properties and use those as a guideline to design desired transport behavior. Fundamentally, this is because the structural and electronic changes manifest at those interfaces have remained hidden from examination. We provide experimental evidence that transport behavior in nanocrystal-in-matrix (NIM) composites is dictated primarily by interfacial charge transfer associated with electronic and structural reconstructions as the composite forms. Our approach building continuous composite superlattices serves as a starting point for systematic probing of the nanointerface of NIM composites via ultrathin films. A combination of field effect transistor device characterization and photoemission spectroscopy reveals the systematic dependence of the polarity of charge transfer on the selection of matrix materials in NIM composites. We use this insight to combine, by design, different components to tune the carrier type in NIM composites.},
doi = {10.1021/acs.chemmater.7b04689},
journal = {Chemistry of Materials},
number = 8,
volume = 30,
place = {United States},
year = {2018},
month = {4}
}