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Register a new userThe role of spin and angular momentum in strong-field ionization
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The spin polarization of electrons from multiphoton ionization of Xe by 395 nm circularly polarized laser pulses at $6cdot10^{13}$ W/cm$^2$ has been measured. At this photon energy of 3.14 eV the above threshold ionization peaks connected to Xe$^+$ ions in the ground state ($J=3/2$, ionization potential $I_p=12.1$ eV) and the first exicted state ($J=1/2$, $I_p=13.4$ eV) are clearly separated in the electron energy distribution. These two combs of ATI peaks show opposite spin polarizations. The magnitude of the spin polarization is a factor of two higher for the $J=1/2$ than for the $J=3/2$ final ionic state. In turn the data show that the ionization probability is strongly dependent on the sign of the magnetic quantum number.
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The combination of photoelectron spectroscopy and ultrafast light sources is on track to set new standards for detailed interrogation of dynamics and reactivity of molecules. A crucial prerequisite for further progress is the ability to not only detect the electron kinetic energy, as done in traditional photoelectron spectroscopy, but also the photoelectron angular distributions (PADs) in the molecular frame. Here carbonylsulfide (OCS) and benzonitrile molecules, fixed in space by combined laser and electrostatic fields, are ionized with intense, circularly polarized, 30 femtosecond laser pulses. For 1-dimensionally oriented OCS the molecular frame PADs exhibit pronounced anisotropies, perpendicular to the fixed permanent dipole moment, that are absent in PADs from randomly oriented molecules. For 3-dimensionally oriented benzonitrile additional striking structures appear due to suppression of electron emission in nodal planes of the fixed electronic orbitals. Our theoretical analysis, relying on tunneling ionization theory, shows that the PADs reflect nodal planes, permanent dipole moments and polarizabilities of both the neutral molecule and its cation. The calculated results are exponentially sensitive to changes in these molecular properties thereby pointing to exciting opportunities for time-resolved probing of valence electrons dynamics by intense circularly polarized pulses. Molecular frame PADs from oriented molecules will prove important in other contexts notably in emerging free-electron-laser studies where localized inner shell electrons are knocked off by x-ray pulses.
Interaction of a strong laser pulse with matter transfers not only energy but also linear momentum of the photons. Recent experimental advances have made it possible to detect the small amount of linear momentum delivered to the photoelectrons in strong-field ionization of atoms. We present numerical simulations as well as an analytical description of the subcycle phase (or time) resolved momentum transfer to an atom accessible by an attoclock protocol. We show that the light-field-induced momentum transfer is remarkably sensitive to properties of the ultrashort laser pulse such as its carrier-envelope phase and ellipticity. Moreover, we show that the subcycle resolved linear momentum transfer can provide novel insights into the interplay between nonadiabatic and nondipole effects in strong-field ionization. This work paves the way towards the investigation of the so-far unexplored time-resolved nondipole nonadiabatic tunneling dynamics.
The problem of time delay in tunneling ionization is revisited. The origin of time delay at the tunnel exit is analysed, underlining the two faces of the concept of the tunnelling time delay: the time delay around the tunnel exit and the asymptotic time delay at a detector. We show that the former time delay, in the sense of a delay in the peak of the wavefunction, exists as a matter of principle and arises due to the sub-barrier interference of the reflected and transmitted components of the tunneling electronic wavepacket. We exemplify this by describing the tunnelling ionization of an electron bound by a short-range potential within the strong field approximation in a deep tunnelling regime. If sub-barrier reflections are extracted from this wavefunction, then the time delay of the peak is shown to vanish. Thus, we assert that the disturbance of the tunnelling wavepacket by the reflection from the surface of the barrier causes a time delay in the neighbourhood of the tunnel exit.
We investigate the helium dimer in strong magnetic fields, focusing on the spectrum of low-lying electronic states and their dissociation curves, at the full configuration-interaction level of theory. To address the loss of cylindrical symmetry and angular momentum as a good quantum number for nontrivial angles between the bond axis and magnetic field, we introduce the almost quantized angular momentum (AQAM) and show that it provides useful information about states in arbitrary orientations. In general, strong magnetic fields dramatically rearrange the spectrum, with the orbital Zeeman effect bringing down states of higher angular momentum below the states with pure $sigma$ character as the field strength increases. In addition, the spin Zeeman effect pushes triplet states below the lowest singlet; in particular, a field of one atomic unit is strong enough to push a quintet state below the triplets. In general, the angle between the bond axis and the magnetic field also continuously modulates the degree of $sigma$, $pi$, and $delta$ character of bonds and the previously identified perpendicular paramagnetic bonding mechanism is found to be common among excited states. Electronic states with preferred skew field orientations are identified and rationalized in terms of permanent and induced electronic currents.
We analyze how bound-state excitation, electron exchange and the residual binding potential influence above-threshold ionization (ATI) in Helium prepared in an excited $p$ state, oriented parallel and perpendicular to a linearly polarized mid-IR field. Using ab initio B-spline Algebraic Diagrammatic Construction (ADC), and several one-electron methods with effective potentials, including the Schrodinger solver Qprop, modifi
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