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Title: Inverse Temperature Dependence of Charge Carrier Hopping in Quantum Dot Solids

Abstract

In semiconductors, increasing mobility with decreasing temperature is a signature of charge carrier transport through delocalized bands. We show that this behavior can also occur in nanocrystal solids due to temperature-dependent structural transformations. Using a combination of broadband infrared transient absorption spectroscopy and numerical modeling, we investigate the temperature-dependent charge transport properties of well-ordered PbS quantum dot (QD) solids. Contrary to expectations, we observe that the QD-to-QD charge tunneling rate increases with decreasing temperature, while simultaneously exhibiting thermally activated nearest-neighbor hopping behavior. Using synchrotron grazing-incidence small-angle X-ray scattering, we show that this trend is driven by a temperature-dependent reduction in nearest-neighbor separation that is quantitatively consistent with the measured tunneling rate.

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [1]
+ Show Author Affiliations
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemical Engineering
  2. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  3. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division
OSTI Identifier:
1476294
Report Number(s):
BNL-209129-2018-JAAM
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
SC0012704; SC0010538
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 12; Journal Issue: 8; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; lead sulfide; nanocrystal; superlattice; temperature-dependent transport; thermal expansion; transient absorption

Citation Formats

Gilmore, Rachel H., Winslow, Samuel W., Lee, Elizabeth M. Y., Ashner, Matthew Nickol, Yager, Kevin G., Willard, Adam P., and Tisdale, William A. Inverse Temperature Dependence of Charge Carrier Hopping in Quantum Dot Solids. United States: N. p., 2018. Web. doi:10.1021/acsnano.8b01643.
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Gilmore, Rachel H., Winslow, Samuel W., Lee, Elizabeth M. Y., Ashner, Matthew Nickol, Yager, Kevin G., Willard, Adam P., & Tisdale, William A. Inverse Temperature Dependence of Charge Carrier Hopping in Quantum Dot Solids. United States. https://doi.org/10.1021/acsnano.8b01643
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Gilmore, Rachel H., Winslow, Samuel W., Lee, Elizabeth M. Y., Ashner, Matthew Nickol, Yager, Kevin G., Willard, Adam P., and Tisdale, William A. Thu . "Inverse Temperature Dependence of Charge Carrier Hopping in Quantum Dot Solids". United States. https://doi.org/10.1021/acsnano.8b01643. https://www.osti.gov/servlets/purl/1476294.
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@article{osti_1476294,
title = {Inverse Temperature Dependence of Charge Carrier Hopping in Quantum Dot Solids},
author = {Gilmore, Rachel H. and Winslow, Samuel W. and Lee, Elizabeth M. Y. and Ashner, Matthew Nickol and Yager, Kevin G. and Willard, Adam P. and Tisdale, William A.},
abstractNote = {In semiconductors, increasing mobility with decreasing temperature is a signature of charge carrier transport through delocalized bands. We show that this behavior can also occur in nanocrystal solids due to temperature-dependent structural transformations. Using a combination of broadband infrared transient absorption spectroscopy and numerical modeling, we investigate the temperature-dependent charge transport properties of well-ordered PbS quantum dot (QD) solids. Contrary to expectations, we observe that the QD-to-QD charge tunneling rate increases with decreasing temperature, while simultaneously exhibiting thermally activated nearest-neighbor hopping behavior. Using synchrotron grazing-incidence small-angle X-ray scattering, we show that this trend is driven by a temperature-dependent reduction in nearest-neighbor separation that is quantitatively consistent with the measured tunneling rate.},
doi = {10.1021/acsnano.8b01643},
journal = {ACS Nano},
number = 8,
volume = 12,
place = {United States},
year = {Thu Jun 21 00:00:00 EDT 2018},
month = {Thu Jun 21 00:00:00 EDT 2018}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1021/acsnano.8b01643
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Cited by: 29 works
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Figures / Tables:

Figure 1 Figure 1: (a) Room-temperature ground state absorption spectra of the three QD batches used in this study. (b-d) Transient absorption (TA) data for the 5.0 nm QDs at 300 K. (c) TA bleach peak energy plotted as a function of time for several sample temperatures. (d) The same data plottedmore » as a change in peak energy relative to zero delay time. The colors used for each temperature are consistent with panel (c).« less
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    Works referencing / citing this record:

    Dependence of stability and electronic and optical properties of perovskite quantum dots on capping ligand chain length
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    • The Journal of Chemical Physics, Vol. 152, Issue 3
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    Nanocrystal superlattices as phonon-engineered solids and acoustic metamaterials
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    Nanocrystal superlattices as phonon-engineered solids and acoustic metamaterials
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