Document Detail


Pulse-induced nonequilibrium dynamics of acetylene inside carbon nanotube studied by an ab initio approach.
MedLine Citation:
PMID:  22615352     Owner:  NLM     Status:  MEDLINE    
Abstract/OtherAbstract:
Nanoscale molecular confinement substantially modifies the functionality and electronic properties of encapsulated molecules. Many works have approached this problem from the perspective of quantifying ground-state molecular changes, but little is known about the nonequilibrium dynamics of encapsulated molecular system. In this letter, we report an analysis of the nonequilibrium dynamics of acetylene (C(2)H(2)) inside a semiconducting carbon nanotube (CNT). An ultrashort high-intense laser pulse (2 fs width and 10(15) W/cm(2) intensity) brings the systems out of equilibrium. This process is modeled by comprehensive first-principles time-dependent density-functional simulations. When encapsulated, acetylene dimer, unlike a single acetylene molecule, exhibits correlated vibrational dynamics (C-C bond rotation and H-C-C bending) that is markedly different from the dynamics observed in the gas phase. This result highlights the role of CNT in modulating the optical electric field within the tube. At longer simulation timescales (> 20 fs) in the largest-diameter tube studied here [CNT(14,0)], we observe synchronized rotation about the C-C axes in the dimer and ultimately ejection of one of the four hydrogen atoms. Our results illustrate the richness of photochemical phenomena in confined geometries.
Authors:
Yoshiyuki Miyamoto; Hong Zhang; Angel Rubio
Publication Detail:
Type:  Journal Article; Research Support, Non-U.S. Gov't     Date:  2012-05-21
Journal Detail:
Title:  Proceedings of the National Academy of Sciences of the United States of America     Volume:  109     ISSN:  1091-6490     ISO Abbreviation:  Proc. Natl. Acad. Sci. U.S.A.     Publication Date:  2012 Jun 
Date Detail:
Created Date:  2012-06-06     Completed Date:  2012-08-27     Revised Date:  2013-06-24    
Medline Journal Info:
Nlm Unique ID:  7505876     Medline TA:  Proc Natl Acad Sci U S A     Country:  United States    
Other Details:
Languages:  eng     Pagination:  8861-5     Citation Subset:  IM    
Affiliation:
National Institute of Advanced Industrial Science and Technology, Central 2, 1-1-1 Umezono, Tsukuba 305-8568, Japan. yoshi-miyamoto@aist.go.jp.
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MeSH Terms
Descriptor/Qualifier:
Acetylene / chemistry*
Dimerization
Electromagnetic Fields
Lasers*
Models, Chemical*
Molecular Dynamics Simulation
Nanotubes, Carbon / chemistry*
Photochemistry
Semiconductors*
Chemical
Reg. No./Substance:
0/Nanotubes, Carbon; 74-86-2/Acetylene
Comments/Corrections

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