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Register a new userAtomic excitation during recollision-free ultrafast multi-electron tunnel ionization
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Modern intense ultrafast pulsed lasers generate an electric field of sufficient strength to permit tunnel ionization of the valence electrons in atoms. This process is usually treated as a rapid succession of isolated events, in which the states of the remaining electrons are neglected. Such electronic interactions are predicted to be weak, the exception being recollision excitation and ionization caused by linearly-polarized radiation. In contrast, it has recently been suggested that intense field ionization may be accompanied by a two-stage `shake-up reaction. Here we report a unique combination of experimental techniques that enables us to accurately measure the tunnel ionization probability for argon exposed to 50 femtosecond laser pulses. Most significantly for the current study, this measurement is independent of the optical focal geometry, equivalent to a homogenous electric field. Furthermore, circularly-polarized radiation negates recollision. The present measurements indicate that tunnel ionization results in simultaneous excitation of one or more remaining electrons through shake-up. From an atomic physics standpoint, it may be possible to induce ionization from specific states, and will influence the development of coherent attosecond XUV radiation sources. Such pulses have vital scientific and economic potential in areas such as high-resolution imaging of in-vivo cells and nanoscale XUV lithography.
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The probability of multiple ionization of krypton by 50 femtosecond circularly polarized laser pulses, independent of the optical focal geometry, has been obtained for the first time. The excellent agreement over the intensity range 10 TWcm-2 to 10 PWcm-2 with the recent predictions of A. S. Kornev et al [Phys. Rev. A v.68, art.043414 (2003)] provides the first experimental confirmation that non-recollisional electronic excitation can occur in strong field ionization. This is particularly true for higher stages of ionization, when the laser intensity exceeds 1 PWcm-2 as the energetic departure of the ionized electron(s) diabatically distorts the wavefunctions of the bound electrons. By scaling the probability of ionization by the focal volume, we discusses why this mechanism was not apparent in previous studies.
Molecules are many body systems with a substantial amount of entanglement between their electrons. Is there a way to break the molecular bond of a diatomic molecule and obtain two atoms in their ground state which are still entangled and form a Bell-like state? We present a scheme that allows for the preparation of such entangled atomic states from single oxygen molecules on femtosecond time scales. The two neutral oxygen atoms are entangled in the magnetic quantum number of their valence electrons. In a time-delayed probe step, we employ non-adiabatic tunnel ionization, which is a magnetic quantum number-sensitive mechanism. We then investigate correlations by comparing single and double ionization probabilities of the Bell-like state. The experimental results agree with the predictions for an entangled state.
Consensus has been reached that recollision, as the most important post-tunneling process, is responsible for nonsequential double ionization process in intense infrared laser field, however, its effect has been restricted to interaction between the first ionized electron and the residual univalent ion so far. Here we identify the key role of recollision between the second ionized electron and the divalent ion in the below-threshold nonsequential double ionization process by introducing a Coulomb-corrected quantum-trajectories method, which enables us to well reproduce the experimentally observed cross-shaped and anti-correlated patterns in correlated two-electron momentum distributions, and also the transition between these two patterns. Being significantly enhanced relatively by the recapture process, recolliding trajectories of the second electron excited by the first- or third-return recolliding trajectories of the first electron produce the cross-shaped or anti-correlated distributions, respectively. And the transition is induced by the increasing contribution of the third return with increasing pulse duration. Our work provides new insight into atomic ionization dynamics and paves the new way to imaging of ultrafast dynamics of atoms and molecules in intense laser field.
The importance of multi-electron dynamics during the tunnel ionization of a correlated quantum system is investigated. By comparison of the solution of the time-dependent Schru007fodinger equation (TDSE) with the time-dependent configuration interaction singles approach (TDCIS), we demonstrate the importance of a multi-electron description of the tunnel ionization process especially for weakly confined quantum systems. Within this context, we observe that adiabatic driving by an intense light field can even enhance the correlations between still trapped electrons.
Hartree-Fock atom in a strong electric static field is considered. It is demonstrated that exchange between outer and inner electrons, taken into account by the so-called Fock term affects strongly the long-range behavior of the inner electron wave function. As a result, it dramatically increases its probability to be ionized. A simple model is analyzed demonstrating that the decay probability, compared to the case of a local (Hartree) atomic potential, increases by many orders of magnitude. As a result of such increase, the ratio of inner to outer electrons ionization probability became not too small. It is essential that the effect of exchange upon probability of inner electron ionization by strong electric field is proportional to the square of the number of outer electrons. It signals that in clusters the inner electron ionization by strong field, the very fact of which is manifested by e.g. high energy quanta emission, has to be essentially increased as compared to this process in gaseous atomic objects.
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