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Akagi, Hiroshi; Otobe, Tomohito; Staudte, A.*; Shiner, A.*; Turner, F.*; D
rner, 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.
Akagi, Hiroshi; Arissian, L.*; Bertrand, J. B.*; Corkum, P. B.*; Gertsvolf, M.*; Pavicic, D.*; Rayner, D. M.*; Smeenk, C.*; Staudte, A.*; Villeneuve, D. M.*; et al.
Laser Physics, 19(8), p.1697 - 1704, 2009/08
Times Cited Count：4 Percentile：25.47(Optics)The paper is divided into four sections. In the first, using atomic ionization as the example, we describe how we can make measurements without re-collision. In the second section we show one approach to measuring the tunnelling probability as a function of molecular alignment using a correlation method. The third section concentrates on how small molecules can be aligned with short laser pulses. Once molecules can be aligned, we can also measure the tunnelling rate as a function of alignment by measuring the ionization probability with linearly polarized light. We use Br
and N as examples. Finally we complete the circle, returning to solids. A traditional STM is confined to the surface of solids. Laser radiation does not suffer from this limitation in large band gap materials. One might expect that the ionization probability would change as a function of the angle between the light polarization and the crystal axis much as it does for a molecule. We complete our review by demonstrating that tunnelling can be used to identify the symmetry of a crystal - with micron spatial precision - anywhere in the bulk.
molecules in intense laser pulsesStaudte, A.*; Patchkovskii, S.*; Pavi
i
, D.*; Akagi, Hiroshi; Smirnova, O.*; Zeidler, D.*; Meckel, M.*; Villeneuve, D. M.*; Drner, R.*; Ivanov, M. Yu.*; et al.
Physical Review Letters, 102(3), p.033004_1 - 033004_4, 2009/01
Times Cited Count：120 Percentile：95.16(Physics, Multidisciplinary)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/HOMO
10
. 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
