N-doping and coalescence of carbon nanotubes: Synthesis and electronic properties

Mauricio Terrones Maldonado, P. M. Ajayan, F. Banhart, X. Blase, D. L. Carroll, J. C. Charlier, R. Czerw, B. Foley, N. Grobert, R. Kamalakaran, P. Kohler-Redlich, M. Rühle, T. Seeger, H. Terrones

Research output: Contribution to journalArticle

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Abstract

Self-assembly pyrolytic routes to large arrays (< 2.5 cm 2 ) of aligned CN x nanotubes (15-80 nm OD and < 100 μm in length) are presented. The method involves the thermolysis of ferrocene/melamine mixtures (5 : 95) at 900-1000 °C in the presence of Ar. Electron energy loss spectroscopy (EELS) reveals that the N content varies from 2%-10%, and can be bonded to C in two different fashions (double-bonded and triple-bonded nitrogen). The electronic densities of states (DOS) of these CN x nanotubes, using scanning tunneling spectroscopy (STS), are presented. The doped nanotubes exhibit strong features in the conduction band close to the Fermi level (0.18 eV). Using tight-binding and ab initio calculations, we confirm that pyridine-like (double-bonded) N is responsible for introducing donor states close to the Fermi Level. These electron-rich structures are the first example of n-type nanotubes. Finally, it will be shown that moderate electron irradiation at 700-800 °C is capable of coalescing single-walled nanotubes (SWNTs). The process has also been studied using tight-binding molecular dynamics (TBMD). Vacancies induce the coalescence via a zipper-like mechanism, which has also been observed experimentally. These vacancies trigger the organization of atoms on the tube lattices within adjacent tubes. These results pave the way to the fabrication of nanotube heterojunctions, robust composites, contacts, nanocircuits and strong 3D composites using i N-doped tubes as well as SWNTs.

Original languageEnglish (US)
Pages (from-to)355-361
Number of pages7
JournalApplied Physics A: Materials Science and Processing
Volume74
Issue number3
DOIs
StatePublished - Mar 1 2002

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Carbon Nanotubes
Coalescence
Electronic properties
Nanotubes
Carbon nanotubes
Doping (additives)
Fermi level
Vacancies
Thermolysis
Electronic density of states
Melamine
Electron irradiation
Electron energy loss spectroscopy
Fasteners
Composite materials
Conduction bands
Pyridine
Self assembly
Heterojunctions
Molecular dynamics

All Science Journal Classification (ASJC) codes

  • Chemistry(all)
  • Materials Science(all)

Cite this

Terrones Maldonado, Mauricio ; Ajayan, P. M. ; Banhart, F. ; Blase, X. ; Carroll, D. L. ; Charlier, J. C. ; Czerw, R. ; Foley, B. ; Grobert, N. ; Kamalakaran, R. ; Kohler-Redlich, P. ; Rühle, M. ; Seeger, T. ; Terrones, H. / N-doping and coalescence of carbon nanotubes : Synthesis and electronic properties. In: Applied Physics A: Materials Science and Processing. 2002 ; Vol. 74, No. 3. pp. 355-361.
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abstract = "Self-assembly pyrolytic routes to large arrays (< 2.5 cm 2 ) of aligned CN x nanotubes (15-80 nm OD and < 100 μm in length) are presented. The method involves the thermolysis of ferrocene/melamine mixtures (5 : 95) at 900-1000 °C in the presence of Ar. Electron energy loss spectroscopy (EELS) reveals that the N content varies from 2{\%}-10{\%}, and can be bonded to C in two different fashions (double-bonded and triple-bonded nitrogen). The electronic densities of states (DOS) of these CN x nanotubes, using scanning tunneling spectroscopy (STS), are presented. The doped nanotubes exhibit strong features in the conduction band close to the Fermi level (0.18 eV). Using tight-binding and ab initio calculations, we confirm that pyridine-like (double-bonded) N is responsible for introducing donor states close to the Fermi Level. These electron-rich structures are the first example of n-type nanotubes. Finally, it will be shown that moderate electron irradiation at 700-800 °C is capable of coalescing single-walled nanotubes (SWNTs). The process has also been studied using tight-binding molecular dynamics (TBMD). Vacancies induce the coalescence via a zipper-like mechanism, which has also been observed experimentally. These vacancies trigger the organization of atoms on the tube lattices within adjacent tubes. These results pave the way to the fabrication of nanotube heterojunctions, robust composites, contacts, nanocircuits and strong 3D composites using i N-doped tubes as well as SWNTs.",
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Terrones Maldonado, M, Ajayan, PM, Banhart, F, Blase, X, Carroll, DL, Charlier, JC, Czerw, R, Foley, B, Grobert, N, Kamalakaran, R, Kohler-Redlich, P, Rühle, M, Seeger, T & Terrones, H 2002, 'N-doping and coalescence of carbon nanotubes: Synthesis and electronic properties', Applied Physics A: Materials Science and Processing, vol. 74, no. 3, pp. 355-361. https://doi.org/10.1007/s003390201278

N-doping and coalescence of carbon nanotubes : Synthesis and electronic properties. / Terrones Maldonado, Mauricio; Ajayan, P. M.; Banhart, F.; Blase, X.; Carroll, D. L.; Charlier, J. C.; Czerw, R.; Foley, B.; Grobert, N.; Kamalakaran, R.; Kohler-Redlich, P.; Rühle, M.; Seeger, T.; Terrones, H.

In: Applied Physics A: Materials Science and Processing, Vol. 74, No. 3, 01.03.2002, p. 355-361.

Research output: Contribution to journalArticle

TY - JOUR

T1 - N-doping and coalescence of carbon nanotubes

T2 - Synthesis and electronic properties

AU - Terrones Maldonado, Mauricio

AU - Ajayan, P. M.

AU - Banhart, F.

AU - Blase, X.

AU - Carroll, D. L.

AU - Charlier, J. C.

AU - Czerw, R.

AU - Foley, B.

AU - Grobert, N.

AU - Kamalakaran, R.

AU - Kohler-Redlich, P.

AU - Rühle, M.

AU - Seeger, T.

AU - Terrones, H.

PY - 2002/3/1

Y1 - 2002/3/1

N2 - Self-assembly pyrolytic routes to large arrays (< 2.5 cm 2 ) of aligned CN x nanotubes (15-80 nm OD and < 100 μm in length) are presented. The method involves the thermolysis of ferrocene/melamine mixtures (5 : 95) at 900-1000 °C in the presence of Ar. Electron energy loss spectroscopy (EELS) reveals that the N content varies from 2%-10%, and can be bonded to C in two different fashions (double-bonded and triple-bonded nitrogen). The electronic densities of states (DOS) of these CN x nanotubes, using scanning tunneling spectroscopy (STS), are presented. The doped nanotubes exhibit strong features in the conduction band close to the Fermi level (0.18 eV). Using tight-binding and ab initio calculations, we confirm that pyridine-like (double-bonded) N is responsible for introducing donor states close to the Fermi Level. These electron-rich structures are the first example of n-type nanotubes. Finally, it will be shown that moderate electron irradiation at 700-800 °C is capable of coalescing single-walled nanotubes (SWNTs). The process has also been studied using tight-binding molecular dynamics (TBMD). Vacancies induce the coalescence via a zipper-like mechanism, which has also been observed experimentally. These vacancies trigger the organization of atoms on the tube lattices within adjacent tubes. These results pave the way to the fabrication of nanotube heterojunctions, robust composites, contacts, nanocircuits and strong 3D composites using i N-doped tubes as well as SWNTs.

AB - Self-assembly pyrolytic routes to large arrays (< 2.5 cm 2 ) of aligned CN x nanotubes (15-80 nm OD and < 100 μm in length) are presented. The method involves the thermolysis of ferrocene/melamine mixtures (5 : 95) at 900-1000 °C in the presence of Ar. Electron energy loss spectroscopy (EELS) reveals that the N content varies from 2%-10%, and can be bonded to C in two different fashions (double-bonded and triple-bonded nitrogen). The electronic densities of states (DOS) of these CN x nanotubes, using scanning tunneling spectroscopy (STS), are presented. The doped nanotubes exhibit strong features in the conduction band close to the Fermi level (0.18 eV). Using tight-binding and ab initio calculations, we confirm that pyridine-like (double-bonded) N is responsible for introducing donor states close to the Fermi Level. These electron-rich structures are the first example of n-type nanotubes. Finally, it will be shown that moderate electron irradiation at 700-800 °C is capable of coalescing single-walled nanotubes (SWNTs). The process has also been studied using tight-binding molecular dynamics (TBMD). Vacancies induce the coalescence via a zipper-like mechanism, which has also been observed experimentally. These vacancies trigger the organization of atoms on the tube lattices within adjacent tubes. These results pave the way to the fabrication of nanotube heterojunctions, robust composites, contacts, nanocircuits and strong 3D composites using i N-doped tubes as well as SWNTs.

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