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Title: Probing the Dependence of Electron Transfer on Size and Coverage in Carbon Nanotube–Quantum Dot Heterostructures

Journal Article · · Journal of Physical Chemistry. C
 [1];  [2];  [3];  [3];  [4];  [1];  [5];  [5];  [4];  [3];  [6]
  1. Department of Chemistry, State University of New York at Stony Brook, Stony Brook, New York 11794-3400, United States
  2. Condensed Matter Physics and Materials Sciences Department, Brookhaven National Laboratory, Building 480, Upton, New York 11973, United States
  3. Department of Electrical and Computer Engineering and Birck Nanotechnology Center, Purdue University, West Lafayette, Indiana 47907, United States
  4. Material Measurement Laboratory, National Institute of Standards and Technology, Gaithersburg, Maryland 20889, United States
  5. School of Marine and Atmospheric Sciences, State University of New York at Stony Brook, Stony Brook, New York 11794-5000, United States
  6. Department of Chemistry, State University of New York at Stony Brook, Stony Brook, New York 11794-3400, United States, Condensed Matter Physics and Materials Sciences Department, Brookhaven National Laboratory, Building 480, Upton, New York 11973, United States

As a model system for understanding charge transfer in novel architectural designs for solar cells, double-walled carbon nanotube (DWNT)–CdSe quantum dot (QD) (QDs with average diameters of 2.3, 3.0, and 4.1 nm) heterostructures have been fabricated. The individual nanoscale building blocks were successfully attached and combined using a hole-trapping thiol linker molecule, i.e., 4-mercaptophenol (MTH), through a facile, noncovalent π–π stacking attachment strategy. Transmission electron microscopy confirmed the attachment of QDs onto the external surfaces of the DWNTs. We herein demonstrate a meaningful and unique combination of near-edge X-ray absorption fine structure (NEXAFS) and Raman spectroscopies bolstered by complementary electrical transport measurements in order to elucidate the synergistic interactions between CdSe QDs and DWNTs, which are facilitated by the bridging MTH molecules that can scavenge photoinduced holes and potentially mediate electron redistribution between the conduction bands in CdSe QDs and the C 2p-derived states of the DWNTs. Specifically, we correlated evidence of charge transfer as manifested by (i) changes in the NEXAFS intensities of π* resonance in the C K-edge and Cd M3-edge spectra, (ii) a perceptible outer tube G-band downshift in frequency in Raman spectra, as well as (iii) alterations in the threshold characteristics present in transport data as a function of CdSe QD deposition onto the DWNT surface. Furthermore, the separate effects of (i) varying QD sizes and (ii) QD coverage densities on the electron transfer were independently studied.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
AC02-98CH10886; SC-00112704; SC00112704
OSTI ID:
1414808
Alternate ID(s):
OSTI ID: 1235852
Report Number(s):
BNL-108987-2015-JA
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Vol. 119 Journal Issue: 47; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 21 works
Citation information provided by
Web of Science

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  • Anderson, Nicholas C.; Hendricks, Mark P.; Choi, Joshua J.
  • Journal of the American Chemical Society, Vol. 135, Issue 49, p. 18536-18548 https://doi.org/10.1021/ja4086758
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