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Maximum relative excitation of a specific vibrational mode via optimum laser-pulse duration Xiang Zhou,1,2 Zhibin Lin,2,3 Chenwei Jiang,4,2 Meng Gao,2 and Roland E. Allen2,*
 

Summary: Maximum relative excitation of a specific vibrational mode via optimum laser-pulse duration
Xiang Zhou,1,2 Zhibin Lin,2,3 Chenwei Jiang,4,2 Meng Gao,2 and Roland E. Allen2,*
1Department of Physics, Wuhan University, Wuhan 430072, China
2Department of Physics, Texas A&M University, College Station, Texas 77843, USA
3Renewable Energy Materials Research Science and Engineering Center, and Department of Physics, Colorado School of Mines,
Golden, Colorado 80401, USA
4
Department of Applied Physics, Xi'an Jiaotong University, Xi'an 710049, China
Received 26 January 2010; revised manuscript received 27 May 2010; published 31 August 2010
For molecules and materials responding to femtosecond-scale optical laser pulses, we predict maximum
relative excitation of a Raman-active vibrational mode with period T when the pulse has a full-width-at-half-
maximum duration 0.42T. This result follows from a general analytical model, and is precisely confirmed
by detailed density-functional-based dynamical simulations for C60 and a carbon nanotube, which include
anharmonicity, nonlinearity, no assumptions about the polarizability tensor, and no averaging over rapid oscil-
lations within the pulse. The mode specificity is, of course, best at low temperature and for pulses that are
electronically off-resonance, and the energy deposited in any mode is proportional to the fourth power of the
electric field.
DOI: 10.1103/PhysRevB.82.075433 PACS number s : 78.30.Na, 78.20.Bh, 78.47.J , 78.67.Ch
For a quarter century there has been considerable interest
in optimizing the vibrational response of molecules and ma-

  

Source: Allen, Roland E. - Department of Physics and Astronomy, Texas A&M University

 

Collections: Physics