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Photoelectron spectroscopy in intense laser fields has proven to be a powerful tool for providing detailed insights into molecular structure. The ionizing molecular orbital, however, has not been reconstructed from the photoelectron spectra, mainly due to the fact that its phase information can be hardly extracted. In this work, we propose a method to retrieve the phase information of the ionizing molecular orbital with laser-induced electron tunneling spectroscopy. By analyzing the interference pattern in the photoelectron spectrum, the weighted coefficients and the relative phases of the constituent atomic orbitals for a molecular orbital can be extracted. With this information we reconstruct the highest occupied molecular orbital of N$_2$. Our work provides a reliable and general approach for imaging of molecular orbitals with the photoelectron spectroscopy., Comment: 6 pages, 4 figures, including Supplementary Materials

We report on an experimental and theoretical study of the ionization-fragmentation dynamics of argon dimers in intense few-cycle laser pulses with a tagged carrier-envelope phase. We find that a field-driven electron transfer process from one argon atom across the system boundary to the other argon atom triggers sub-cycle electron-electron interaction dynamics in the neighboring atom. This attosecond electron-transfer process between distant entities and its implications manifest themselves as a distinct phase-shift between the measured asymmetry of electron emission curves of the $\text{Ar}^{+}+\text{Ar}^{2+}$ and $\text{Ar}^{2+}+\text{Ar}^{2+}$ fragmentation channels. Our work discloses a strong-field route to controlling the dynamics in molecular compounds through the excitation of electronic dynamics on a distant molecule by driving inter-molecular electron-transfer processes.

We unambiguously identify, in experiment and theory, a previously overlooked holographic interference pattern in strong-field ionization, dubbed "the spiral", stemming from two trajectories for which the binding potential and the laser field are equally critical. We show that, due to strong interaction with the core, these trajectories are optimal tools for probing the target \textbf{after} ionization and for revealing obfuscated phases in the initial bound states. The spiral is shown to be responsible for interference carpets, formerly attributed to direct above-threshold ionization trajectories, and we show the carpet-interference condition is a general property due to the field symmetry., Comment: 6 pages, 4 figures, 2 tables