Metal-Insulator Transition in Nanoparticle Solids: Insights from Kinetic Monte Carlo Simulations
Abstract
Progress has been rapid in increasing the efficiency of energy conversion in nanoparticles. However, extraction of the photo-generated charge carriers remains challenging. Encouragingly, the charge mobility has been improved recently by driving nanoparticle (NP) films across the metal-insulator transition (MIT). To simulate MIT in NP films, we developed a hierarchical Kinetic Monte Carlo transport model. Electrons transfer between neighboring NPs via activated hopping when the NP energies differ by more than an overlap energy, but transfer by a non-activated quantum delocalization, if the NP energies are closer than the overlap energy. As the overlap energy increases, emerging percolating clusters support a metallic transport across the entire film. We simulated the evolution of the temperature-dependent electron mobility. We analyzed our data in terms of two candidate models of the MIT: (a) as a Quantum Critical Transition, signaled by an effective gap going to zero; and (b) as a Quantum Percolation Transition, where a sample-spanning metallic percolation path is formed as the fraction of the hopping bonds in the transport paths is going to zero. We found that the Quantum Percolation Transition theory provides a better description of the MIT. We also observed an anomalously low gap region next to the MIT.more »
- Authors:
-
[2];
- Univ. of California, Davis, CA (United States)
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States)
- Sponsoring Org.:
- National Science Foundation (NSF); USDOE
- OSTI Identifier:
- 1392500
- Grant/Contract Number:
- AC02-06CH11357
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS
Citation Formats
Qu, Luman, Vörös, Márton, and Zimanyi, Gergely T. Metal-Insulator Transition in Nanoparticle Solids: Insights from Kinetic Monte Carlo Simulations. United States: N. p., 2017.
Web. doi:10.1038/s41598-017-06497-1.
Qu, Luman, Vörös, Márton, & Zimanyi, Gergely T. Metal-Insulator Transition in Nanoparticle Solids: Insights from Kinetic Monte Carlo Simulations. United States. https://doi.org/10.1038/s41598-017-06497-1
Qu, Luman, Vörös, Márton, and Zimanyi, Gergely T. Tue .
"Metal-Insulator Transition in Nanoparticle Solids: Insights from Kinetic Monte Carlo Simulations". United States. https://doi.org/10.1038/s41598-017-06497-1. https://www.osti.gov/servlets/purl/1392500.
@article{osti_1392500,
title = {Metal-Insulator Transition in Nanoparticle Solids: Insights from Kinetic Monte Carlo Simulations},
author = {Qu, Luman and Vörös, Márton and Zimanyi, Gergely T.},
abstractNote = {Progress has been rapid in increasing the efficiency of energy conversion in nanoparticles. However, extraction of the photo-generated charge carriers remains challenging. Encouragingly, the charge mobility has been improved recently by driving nanoparticle (NP) films across the metal-insulator transition (MIT). To simulate MIT in NP films, we developed a hierarchical Kinetic Monte Carlo transport model. Electrons transfer between neighboring NPs via activated hopping when the NP energies differ by more than an overlap energy, but transfer by a non-activated quantum delocalization, if the NP energies are closer than the overlap energy. As the overlap energy increases, emerging percolating clusters support a metallic transport across the entire film. We simulated the evolution of the temperature-dependent electron mobility. We analyzed our data in terms of two candidate models of the MIT: (a) as a Quantum Critical Transition, signaled by an effective gap going to zero; and (b) as a Quantum Percolation Transition, where a sample-spanning metallic percolation path is formed as the fraction of the hopping bonds in the transport paths is going to zero. We found that the Quantum Percolation Transition theory provides a better description of the MIT. We also observed an anomalously low gap region next to the MIT. We discuss the relevance of our results in the light of recent experimental measurements.},
doi = {10.1038/s41598-017-06497-1},
journal = {Scientific Reports},
number = 1,
volume = 7,
place = {United States},
year = {Tue Aug 01 00:00:00 EDT 2017},
month = {Tue Aug 01 00:00:00 EDT 2017}
}
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