Journal
CHEMPHYSCHEM
Volume 14, Issue 7, Pages 1451-1455Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/cphc.201201045
Keywords
1; 3-cyclohexadiene; ab initio calculations; angle-resolved ionization yields; molecular orbitals; strong-field ionization
Funding
- Department of Energy [DE-FG02-08ER15983, DE-FG02-08ER15984]
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We compare the time- and angle-dependent strong-field ionization yields of three molecules with very similar electronic structure. A pump pulse in the deep ultraviolet excites 1,3-cyclohexadiene, -terpinene, and -phellandrene to their first excited state. The latter two molecules are alkyl-substituted 1,3-cyclohexadiene systems. We then measure the strong-field ionization yield due to a near infrared probe pulse as a function of delay and angle between pump and probe polarization vectors. Ab initio electronic structure calculations allow us to associate the parent ion yields with removal of an electron from a LUMO orbital (occupied after excitation by the pump). Despite the fact that the LUMO orbitals for these molecules are very similar, the angle-dependent yields are very different, indicating that it is not the orbital shape alone which determines angle-dependent ionization yields.
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