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Pulse-induced nonequilibrium dynamics of acetylene inside carbon nanotube studied by an ab initio approach
Yoshiyuki Miyamoto, Hong Zhang and Angel Rubio
Proceedings of the National Academy of Sciences of the United States of America
Vol. 109, No. 23 (June 5, 2012), pp. 8861-8865
Published by: National Academy of Sciences
Stable URL: http://www.jstor.org/stable/41603017
Page Count: 5
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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 (C₂H₂) inside a semiconducting carbon nanotube (CNT). An ultrashort high-intense laser pulse (2 fs width and 10¹⁵ W/cm² 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.
Proceedings of the National Academy of Sciences of the United States of America © 2012 National Academy of Sciences