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Akagi, Hiroshi; Otobe, Tomohito; Staudte, A.*; Shiner, A.*; Turner, F.*; Drner, R.*; Villeneuve, D. M.*; Corkum, P. B.*
Science, 325(5946), p.1364 - 1367, 2009/09
Times Cited Count:273 Percentile:98.68(Multidisciplinary Sciences)Tunneling, one of the most striking manifestations of quantum mechanics, influences the electronic structure of many molecules and solids and is responsible for radioactive decay. Much of the interaction of intense light pulses with matter commences with electrons tunneling from atoms or molecules to the continuum. Until recently, this starting point was assumed to be the highest occupied orbital of a given system. Here, we report the observation of tunneling from a lower lying state in HCl. Analyzing two independent experimental observables allows us to isolate (via fragment ions), identify (via molecular frame photoelectron angular distributions) and, with the help of ab-initio simulations, quantify the contribution of lower lying orbitals to the total and angle dependent tunneling current of the molecule.
Boucher, D.*; Connor, J. W.*; Houlberg, W. A.*; Turner, M. F.*; Bracco, G.*; Chudnovskiy, A.*; Cordey, J. G.*; Greenwald, M. J.*; Hoang, G. T.*; Hogeweij, G. M. D.*; et al.
Nuclear Fusion, 40(12), p.1955 - 1981, 2000/12
no abstracts in English
Akagi, Hiroshi; Staudte, A.*; Shiner, A.*; Turner, F.*; Villeneuve, D. M.*; Corkum, P. B.*
no journal, ,
For homogeneous molecules, experiments show tunneling projects a filtered version of an orbital to the continuum. Ours are the first measurements for a heteronuclear molecule. To determine the angle, we use circularly polarized light and measure the electron and fragment ion in coincidence. Concentrating on HCl, we find that the branching ratio for tunneling is HOMO-1/HOMO10. The angle dependent tunnelling probability for the HOMO-1 reflects the shape of the orbital.
Akagi, Hiroshi; Staudte, A.*; Shiner, A.*; Turner, F.*; Villeneuve, D. M.*; Ivanov, M. Yu.*; Corkum, P. B.*
no journal, ,
Angular dependence of tunnel ionization from a molecule in a strong laser field reflects the structure of the molecular orbital the electron tunnels from. Ours are the first measurements for a heteronuclear molecule. To determine the angle, we use circularly polarized light and detect the electron and fragment ion in coincidence. Concentrating on HCl, bond softening allows us to select the tunnel ionization from HOMO-1. The angular distribution is consistent with the shape of the orbital, modified by a contribution from the dipole moment of the neutral molecule and its cation.
Akagi, Hiroshi; Otobe, Tomohito; Staudte, A.*; Shiner, A.*; Turner, F.*; Villeneuve, D. M.*; Doerner, R.*; Corkum, P. B.*
no journal, ,
no abstracts in English
Akagi, Hiroshi; Otobe, Tomohito; Staudte, A.*; Shiner, A.*; Villeneuve, D. M.*; Corkum, P. B.*; Turner, F.*; Doerner, R.*
no journal, ,
no abstracts in English