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Issue 18, 2012
From the journal:

Physical Chemistry Chemical Physics

Time-dependent quantum dynamical simulations of C2 condensation under extreme conditions

Jacek Jakowski,*a   Stephan Irleb  and  Keiji Morokumacd  

* Corresponding authors

a National Institute for Computational Sciences, Oak Ridge, Tennessee 37831, USA
E-mail: jjakowsk@utk.edu

b Institute for Advanced Research and Department of Chemistry, Nagoya University, Nagoya 464-8602, Japan

c Cherry L. Emerson Center for Scientific Computation and Department of Chemistry, Emory University, 1515 Dickey Drive, Atlanta, Georgia 30322, USA

d Fukui Institute for Fundamental Chemistry, Kyoto University, Sakyo, Kyoto 6006-8103, Japan

Abstract

We report theoretical studies of the initial phase of bulk C2 condensation into carbon nano-structures by means of Born–Oppenheimer and time-dependent quantum mechanical Liouville–von Neumann molecular dynamics based on the density-functional tight-binding (DFTB) framework for electrons. We observe that the time-dependent quantum mechanical approach leads to faster formation of carbon nanostructures than analogous Born–Oppenheimer simulations. Our results suggest that the condensation of bulk carbon is nonadiabatic in nature, with the critical role of electronic stopping as in ion-irradiation of materials. Contrary to time-dependent quantum mechanical simulations, Born–Oppenheimer dynamics incorrectly predict that the short carbon chains obtained from initial reactive collisions between C2 quickly evaporate, leading to much lower probability of secondary collisions and condensation. We also discuss some deficiencies in Born–Oppenheimer dynamics that lead to unphysical charge polarization and electron transfer.

Graphical abstract: Time-dependent quantum dynamical simulations of C2 condensation under extreme conditions

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Article information

DOI
https://doi.org/10.1039/C1CP22035G
Article type
Paper
Submitted
22 Jun 2011
Accepted
08 Nov 2011
First published
07 Dec 2011

Phys. Chem. Chem. Phys., 2012,14, 6273-6279

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Time-dependent quantum dynamical simulations of C2 condensation under extreme conditions

J. Jakowski, S. Irle and K. Morokuma, Phys. Chem. Chem. Phys., 2012, 14, 6273 DOI: 10.1039/C1CP22035G

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