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Title: Negligible Electronic Interaction between Photoexcited Electron–Hole Pairs and Free Electrons in Phosphorus–Boron Co-Doped Silicon Nanocrystals

Phosphorus (P) and boron (B) co-doped Si nanocrystals (NCs) have raised interest in the optoelectronic industry due to their electronic tunability, optimal carrier multiplication properties, and straightforward dispersibility in polar solvents. Yet a basic understanding of the interaction of photoexcited electron-hole (e-h) pairs with new physical features that are introduced by the co-doping process (free carriers, defect states, and surface chemistry) is missing. Here, we present the first study of the ultrafast carrier dynamics in SiO2-embedded P-B co-doped Si NC ensembles using induced absorption spectroscopy through a two-step approach. First, the induced absorption data show that the large fraction of the dopants residing on the NC surface slows down carrier relaxation dynamics within the first 20 ps relative to intrinsic (undoped) Si NCs, which we interpret as enhanced surface passivation. On longer time-scales (picosecond to nanosecond regime), we observe a speeding up of the carrier relaxation dynamics and ascribe it to doping-induced trap states. This argument is deduced from the second part of the study, where we investigate multiexciton interactions. From a stochastic modeling approach we show that localized carriers, which are introduced by the P or B dopants, have minor electronic interactions with the photoexcited e-h pairs. This ismore » understood in light of the strong localization of the introduced carriers on their original P- or B-dopant atoms, due to the strong quantum confinement regime in these relatively small NCs (<6 nm).« less
Authors:
ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [1] ; ORCiD logo [3]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Kobe Univ. (Japan)
  3. Univ. of Amsterdam (Netherlands)
Publication Date:
Report Number(s):
NREL/JA-5900-70658
Journal ID: ISSN 1932-7447
Grant/Contract Number:
AC36-08GO28308; AC36- 08GO28308
Type:
Published Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 122; Journal Issue: 11; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY; 36 MATERIALS SCIENCE; ultrafast; phosphorous-boron; nanocrystals
OSTI Identifier:
1427876
Alternate Identifier(s):
OSTI ID: 1435709

Limpens, Rens, Fujii, Minoru, Neale, Nathan R., and Gregorkiewicz, Tom. Negligible Electronic Interaction between Photoexcited Electron–Hole Pairs and Free Electrons in Phosphorus–Boron Co-Doped Silicon Nanocrystals. United States: N. p., Web. doi:10.1021/acs.jpcc.7b12313.
Limpens, Rens, Fujii, Minoru, Neale, Nathan R., & Gregorkiewicz, Tom. Negligible Electronic Interaction between Photoexcited Electron–Hole Pairs and Free Electrons in Phosphorus–Boron Co-Doped Silicon Nanocrystals. United States. doi:10.1021/acs.jpcc.7b12313.
Limpens, Rens, Fujii, Minoru, Neale, Nathan R., and Gregorkiewicz, Tom. 2018. "Negligible Electronic Interaction between Photoexcited Electron–Hole Pairs and Free Electrons in Phosphorus–Boron Co-Doped Silicon Nanocrystals". United States. doi:10.1021/acs.jpcc.7b12313.
@article{osti_1427876,
title = {Negligible Electronic Interaction between Photoexcited Electron–Hole Pairs and Free Electrons in Phosphorus–Boron Co-Doped Silicon Nanocrystals},
author = {Limpens, Rens and Fujii, Minoru and Neale, Nathan R. and Gregorkiewicz, Tom},
abstractNote = {Phosphorus (P) and boron (B) co-doped Si nanocrystals (NCs) have raised interest in the optoelectronic industry due to their electronic tunability, optimal carrier multiplication properties, and straightforward dispersibility in polar solvents. Yet a basic understanding of the interaction of photoexcited electron-hole (e-h) pairs with new physical features that are introduced by the co-doping process (free carriers, defect states, and surface chemistry) is missing. Here, we present the first study of the ultrafast carrier dynamics in SiO2-embedded P-B co-doped Si NC ensembles using induced absorption spectroscopy through a two-step approach. First, the induced absorption data show that the large fraction of the dopants residing on the NC surface slows down carrier relaxation dynamics within the first 20 ps relative to intrinsic (undoped) Si NCs, which we interpret as enhanced surface passivation. On longer time-scales (picosecond to nanosecond regime), we observe a speeding up of the carrier relaxation dynamics and ascribe it to doping-induced trap states. This argument is deduced from the second part of the study, where we investigate multiexciton interactions. From a stochastic modeling approach we show that localized carriers, which are introduced by the P or B dopants, have minor electronic interactions with the photoexcited e-h pairs. This is understood in light of the strong localization of the introduced carriers on their original P- or B-dopant atoms, due to the strong quantum confinement regime in these relatively small NCs (<6 nm).},
doi = {10.1021/acs.jpcc.7b12313},
journal = {Journal of Physical Chemistry. C},
number = 11,
volume = 122,
place = {United States},
year = {2018},
month = {2}
}