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Title: Surface Structure of Aerobically Oxidized Diamond Nanocrystals

Abstract

Here we investigate the aerobic oxidation of high-pressure, high-temperature nanodiamonds (5–50 nm dimensions) using a combination of carbon and oxygen K-edge X-ray absorption, wavelength-dependent X-ray photoelectron, and vibrational spectroscopies. Oxidation at 575 °C for 2 h eliminates graphitic carbon contamination (>98%) and produces nanocrystals with hydroxyl functionalized surfaces as well as a minor component (<5%) of carboxylic anhydrides. The low graphitic carbon content and the high crystallinity of HPHT are evident from Raman spectra acquired using visible wavelength excitation (λ excit = 633 nm) as well as carbon K-edge X-ray absorption spectra where the signature of a core–hole exciton is observed. Both spectroscopic features are similar to those of chemical vapor deposited (CVD) diamond but differ significantly from the spectra of detonation nanodiamond. Lastly, we discuss the importance of these findings to the functionalization of nanodiamond surfaces for biological labeling applications.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5];  [6];  [3];  [7]
  1. Columbia Univ., New York, NY (United States). Dept. of Chemistry; Columbia Univ., New York, NY (United States). Dept. of Electrical Engineering; Columbia Univ., New York, NY (United States). Dept. of Applied Mathematics and Applied Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science; Diamond Nanotechnologies Inc., Boston, MA (United States)
  2. Columbia Univ., New York, NY (United States). Energy Frontier Research Center
  3. Columbia Univ., New York, NY (United States). Dept. of Electrical Engineering; Columbia Univ., New York, NY (United States). Dept. of Applied Mathematics and Applied Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science
  4. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL)
  5. Brookhaven National Lab. (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  6. Columbia Univ., New York, NY (United States). Dept. of Electrical Engineering; Columbia Univ., New York, NY (United States). Dept. of Applied Mathematics and Applied Physics; Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Electrical Engineering and Computer Science; Diamond Nanotechnologies Inc., Boston, MA (United States)
  7. Columbia Univ., New York, NY (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Re-Defining Photovoltaic Efficiency Through Molecule Scale Control (RPEMSC); Brookhaven National Lab. (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1229426
Report Number(s):
BNL-111502-2015-JA
Journal ID: ISSN 1932-7447
Grant/Contract Number:  
SC00112704; W911NF-12-1-0594; SC0001085; AC02-98CH10886; HDTRA1-11-1-0022; HR0011-14-C-0018; D14PC00121; 1R43MH102942-01
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 118; Journal Issue: 46; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Wolcott, Abraham, Schiros, Theanne, Trusheim, Matthew E., Chen, Edward H., Nordlund, Dennis, Diaz, Rosa E., Gaaton, Ophir, Englund, Dirk, and Owen, Jonathan S. Surface Structure of Aerobically Oxidized Diamond Nanocrystals. United States: N. p., 2014. Web. doi:10.1021/jp506992c.
Wolcott, Abraham, Schiros, Theanne, Trusheim, Matthew E., Chen, Edward H., Nordlund, Dennis, Diaz, Rosa E., Gaaton, Ophir, Englund, Dirk, & Owen, Jonathan S. Surface Structure of Aerobically Oxidized Diamond Nanocrystals. United States. doi:10.1021/jp506992c.
Wolcott, Abraham, Schiros, Theanne, Trusheim, Matthew E., Chen, Edward H., Nordlund, Dennis, Diaz, Rosa E., Gaaton, Ophir, Englund, Dirk, and Owen, Jonathan S. Mon . "Surface Structure of Aerobically Oxidized Diamond Nanocrystals". United States. doi:10.1021/jp506992c. https://www.osti.gov/servlets/purl/1229426.
@article{osti_1229426,
title = {Surface Structure of Aerobically Oxidized Diamond Nanocrystals},
author = {Wolcott, Abraham and Schiros, Theanne and Trusheim, Matthew E. and Chen, Edward H. and Nordlund, Dennis and Diaz, Rosa E. and Gaaton, Ophir and Englund, Dirk and Owen, Jonathan S.},
abstractNote = {Here we investigate the aerobic oxidation of high-pressure, high-temperature nanodiamonds (5–50 nm dimensions) using a combination of carbon and oxygen K-edge X-ray absorption, wavelength-dependent X-ray photoelectron, and vibrational spectroscopies. Oxidation at 575 °C for 2 h eliminates graphitic carbon contamination (>98%) and produces nanocrystals with hydroxyl functionalized surfaces as well as a minor component (<5%) of carboxylic anhydrides. The low graphitic carbon content and the high crystallinity of HPHT are evident from Raman spectra acquired using visible wavelength excitation (λexcit = 633 nm) as well as carbon K-edge X-ray absorption spectra where the signature of a core–hole exciton is observed. Both spectroscopic features are similar to those of chemical vapor deposited (CVD) diamond but differ significantly from the spectra of detonation nanodiamond. Lastly, we discuss the importance of these findings to the functionalization of nanodiamond surfaces for biological labeling applications.},
doi = {10.1021/jp506992c},
journal = {Journal of Physical Chemistry. C},
number = 46,
volume = 118,
place = {United States},
year = {2014},
month = {10}
}

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Cited by: 18 works
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