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Title: Fully versus constrained statistical fragmentation of carbon clusters and their heteronuclear derivatives

Abstract

The Microcanonical Metropolis Monte Carlo (MMMC) method has been shown to describe reasonably well fragmentation of clusters composed of identical atomic species. However, this is not so clear in the case of heteronuclear clusters as some regions of phase space might be inaccessible due to the different mobility of the different atomic species, the existence of large isomerization barriers, or the quite different chemical nature of the possible intermediate species. In this paper, we introduce a constrained statistical model that extends the range of applicability of the MMMC method to such mixed clusters. The method is applied to describe fragmentation of isolated clusters with high, moderate, and no heteronuclear character, namely, C nH m, C nN, and C n clusters for which experimental fragmentation branching ratios are available in the literature. We show that the constrained statistical model describes fairly well fragmentation of CnHm clusters in contrast with the poor description provided by the fully statistical model. The latter model, however, works pretty well for both C n and C nN clusters, thus showing that the ultimate reason for this discrepancy is the inability of the MMMC method to selectively explore the whole phase space. This conclusion has driven usmore » to predict the fragmentation patterns of the C 4N cluster for which experiments are not yet available.« less

Authors:
ORCiD logo [1]; ORCiD logo [2];  [3];  [3];  [4];  [5]; ORCiD logo [5]
  1. Univ. Autónoma de Madrid, Madrid (Spain); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. Univ. Autónoma de Madrid, Madrid (Spain)
  3. Univ. Paris-Sud, Orsay (France). Inst. de Physique Nucléaire d’Orsay
  4. Univ. Paris-Sud, Orsay (France). Inst. des Sciences Moléculaires d’Orsay
  5. Univ. Autónoma de Madrid, Madrid (Spain); Inst. Madrileño de Estudios Avanzados en Nanociencia (IMDEA-Nanociencia), Cantoblanco, Madrid (Spain)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
MINECO; USDOE
OSTI Identifier:
1511242
Report Number(s):
LA-UR-18-29010
Journal ID: ISSN 0021-9606
Grant/Contract Number:  
89233218CNA000001
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 150; Journal Issue: 14; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Aguirre, Néstor F., Díaz-Tendero, Sergio, IdBarkach, Tijani, Chabot, Marin, Béroff, Karine, Alcamí, Manuel, and Martín, Fernando. Fully versus constrained statistical fragmentation of carbon clusters and their heteronuclear derivatives. United States: N. p., 2019. Web. doi:10.1063/1.5083864.
Aguirre, Néstor F., Díaz-Tendero, Sergio, IdBarkach, Tijani, Chabot, Marin, Béroff, Karine, Alcamí, Manuel, & Martín, Fernando. Fully versus constrained statistical fragmentation of carbon clusters and their heteronuclear derivatives. United States. doi:10.1063/1.5083864.
Aguirre, Néstor F., Díaz-Tendero, Sergio, IdBarkach, Tijani, Chabot, Marin, Béroff, Karine, Alcamí, Manuel, and Martín, Fernando. Sun . "Fully versus constrained statistical fragmentation of carbon clusters and their heteronuclear derivatives". United States. doi:10.1063/1.5083864.
@article{osti_1511242,
title = {Fully versus constrained statistical fragmentation of carbon clusters and their heteronuclear derivatives},
author = {Aguirre, Néstor F. and Díaz-Tendero, Sergio and IdBarkach, Tijani and Chabot, Marin and Béroff, Karine and Alcamí, Manuel and Martín, Fernando},
abstractNote = {The Microcanonical Metropolis Monte Carlo (MMMC) method has been shown to describe reasonably well fragmentation of clusters composed of identical atomic species. However, this is not so clear in the case of heteronuclear clusters as some regions of phase space might be inaccessible due to the different mobility of the different atomic species, the existence of large isomerization barriers, or the quite different chemical nature of the possible intermediate species. In this paper, we introduce a constrained statistical model that extends the range of applicability of the MMMC method to such mixed clusters. The method is applied to describe fragmentation of isolated clusters with high, moderate, and no heteronuclear character, namely, CnHm, CnN, and Cn clusters for which experimental fragmentation branching ratios are available in the literature. We show that the constrained statistical model describes fairly well fragmentation of CnHm clusters in contrast with the poor description provided by the fully statistical model. The latter model, however, works pretty well for both Cn and CnN clusters, thus showing that the ultimate reason for this discrepancy is the inability of the MMMC method to selectively explore the whole phase space. This conclusion has driven us to predict the fragmentation patterns of the C4N cluster for which experiments are not yet available.},
doi = {10.1063/1.5083864},
journal = {Journal of Chemical Physics},
number = 14,
volume = 150,
place = {United States},
year = {2019},
month = {4}
}

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