Ligand-induced dependence of charge transfer in nanotube–quantum dot heterostructures

Wang, Lei; Han, Jinkyu; Sundahl, Bryan; Thornton, Scott; Zhu, Yuqi; Zhou, Ruiping; Jaye, Cherno; Liu, Haiqing; Li, Zhuo-Qun; Taylor, Gordon T.; Fischer, Daniel A.; Appenzeller, Joerg; Harrison, Robert J.; Wong, Stanislaus S.

doi:10.1039/C6NR03091B

Title: Ligand-induced dependence of charge transfer in nanotube–quantum dot heterostructures

Journal Article · Fri Jul 01 00:00:00 EDT 2016 · Nanoscale

DOI:https://doi.org/10.1039/C6NR03091B· OSTI ID:1303000

Wang, Lei ^[1]; Han, Jinkyu ^[2]; Sundahl, Bryan ^[3]; Thornton, Scott ^[3]; Zhu, Yuqi ^[4]; Zhou, Ruiping ^[4]; Jaye, Cherno ^[5]; Liu, Haiqing ^[1]; Li, Zhuo-Qun ^[6]; Taylor, Gordon T. ^[6]; Fischer, Daniel A. ^[5]; Appenzeller, Joerg ^[4]; Harrison, Robert J. ^[7]; Wong, Stanislaus S. ^[8]

Stony Brook Univ., NY (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Sciences Division
State Univ. of New York (SUNY) at Stony Brook, Stony Brook, NY (United States). Inst. of Advanced Computational Science
Purdue Univ., West Lafayette, IN (United States). Birck Nanotechnology Center, Dept. of Electrical and Computer Engineering
National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). Material Measurement Lab.
State Univ. of New York (SUNY) at Stony Brook, Stony Brook, NY (United States). School of Marine and Atmospheric Sciences
State Univ. of New York (SUNY) at Stony Brook, Stony Brook, NY (United States). Inst. of Advanced Computational Science; Brookhaven National Lab. (BNL), Upton, NY (United States). Computational Science Center
Stony Brook Univ., NY (United States). Dept. of Chemistry; Brookhaven National Lab. (BNL), Upton, NY (United States). Condensed Matter Physics and Materials Sciences Division

As a model system to probe ligand-dependent charge transfer in complex composite heterostructures, we fabricated double-walled carbon nanotube (DWNT) – CdSe quantum dot (QD) composites. Whereas the average diameter of the QDs probed was kept fixed at ~4.1 nm and the nanotubes analyzed were similarly oxidatively processed, by contrast, the ligands used to mediate the covalent attachment between the QDs and DWNTs were systematically varied to include p-phenylenediamine (PPD), 2-aminoethanethiol (AET), and 4-aminothiophenol (ATP). Herein, we have put forth a unique compilation of complementary data from experiment and theory, including results from transmission electron microscopy (TEM), near-edge X-ray absorption fine structure (NEXAFS) spectroscopy, Raman spectroscopy, electrical transport measurements, and theoretical modeling studies, in order to fundamentally assess the nature of the charge transfer between CdSe QDs and DWNTs, as a function of the structure of various, intervening bridging ligand molecules. Specifically, we correlated evidence of charge transfer as manifested by changes and shifts associated with NEXAFS intensities, Raman peak positions, and threshold voltages both before and after CdSe QD deposition onto the underlying DWNT surface. Importantly, for the first time ever in these types of nanoscale composite systems, we have sought to use theoretical modeling to justify and account for our experimental results. Finally, our overall data suggest that (i) QD coverage density on the DWNTs varies, based upon the different ligand pendant groups used and that (ii) the presence of a π-conjugated carbon framework within the ligands themselves and the electron affinity of the pendant groups collectively play important roles in the resulting charge transfer from QDs to the underlying CNTs.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704; ACI-121664; OCE-1336724

OSTI ID:: 1303000

Report Number(s):: BNL-112413-2016-JA; NANOHL; R&D Project: PM037; KC0201030

Journal Information:: Nanoscale, Journal Name: Nanoscale; ISSN 2040-3364

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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charge transfer
CdSe QDs
DWNTs
ligands

Title: Ligand-induced dependence of charge transfer in nanotube–quantum dot heterostructures

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