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 Title: Femtosecond laser studies of molecular wavepacket dynamics in the cesium dimer Author(s): Rodriguez, George Doctoral Committee Chair(s): Eden, James G. Department / Program: Electrical and Computer Engineering Discipline: Electrical Engineering Degree Granting Institution: University of Illinois at Urbana-Champaign Degree: Ph.D. Genre: Dissertation Subject(s): Chemistry, Physical Physics, Molecular Physics, Optics Abstract: Femtosecond laser pump-probe experiments have been applied to the study of vibrational wavepacket dynamics in the excited states of the cesium dimer, Cs$\sb2.$ The real-time vibrational motion of the molecule is observed by probing the quantum motion of the wavepacket on a potential surface by a pair of time-delayed ultrafast laser pulses. Specifically, pumping the $\rm C(\sp1\Pi\sb{u})\gets X(\sp1\Sigma\sb{g}\sp+)\ Cs\sb2$ band at several wavelengths between 627 nm and 650 nm produces a wavepacket with an oscillation period of $\sim$1.15 psec. The wavepacket is detected by photoionizing the excited molecule with a time-delayed probe pulse. The wavepacket oscillations persist for approximately 20 psec, and their decay is attributed to the dephasing of the vibrational wavefunctions that comprise the wavepacket.Using the Fast Fourier Transform (FFT) spectral method, numerical quantum calculations of the time dependent Schrodinger equation have been performed to simulate the time evolution of the wavepacket density. The wavepacket simulations reproduce the experimentally observed oscillations, and can be used to describe the classical motion of the molecule. Issue Date: 1993 Type: Text Language: English URI: http://hdl.handle.net/2142/22033 Rights Information: Copyright 1993 Rodriguez, George Date Available in IDEALS: 2011-05-07 Identifier in Online Catalog: AAI9314931 OCLC Identifier: (UMI)AAI9314931
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