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arXiv:1803.07355 · Nature Communications

Double-slit photoelectron interference in strong-field ionization of the neon dimer

Maksim Kunitski, Nicolas Eicke, Pia Huber, Jonas Köhler, Stefan Zeller, Jörg Voigtsberger, Nikolai Schlott, Kevin Henrichs, Hendrik Sann, Florian Trinter, Lothar Ph. H. Schmidt, Anton Kalinin, Markus S. Schöffler, T. Jahnke, Manfred Lein, Reinhard Dörner

Published Dec 27, 2018• 8,161 citations
arXivHTMLPDF

Abstract

Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.

DOI
10.1038/s41467-018-07882-8

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Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.
Wave-particle duality is an inherent peculiarity of the quantum world. The double-slit experiment has been frequently used for understanding different aspects of this fundamental concept. The occurrence of interference rests on the lack of which-way information and on the absence of decoherence mechanisms, which could scramble the wave fronts. Here, we report on the observation of two-center interference in the molecular-frame photoelectron momentum distribution upon ionization of the neon dimer by a strong laser field. Postselection of ions, which are measured in coincidence with electrons, allows choosing the symmetry of the residual ion, leading to observation of both, gerade and ungerade, types of interference.
In a double-slit experiment with a bipartite system, the visibility of interference fringes depends on the availability of which-way information. Here, we report a Bell-like state of photoelectron and residual ion in the multiphoton dissociative ionization of the D2_22​ molecule. Evidence for entanglement is provided by the correlated emission directions of photoelectron and ion, which is observed using a COLTRIMS reaction microscope. In the presence of this correlation, the holographic interference fringes contained in the photoelectron momentum distributions are suppressed, indicating the existence of which-way information. The interference pattern persists when a single ionic state is populated and thus no which-way information is available. The experimental observations and conclusions are supported by the numerical solution of the electronic-nuclear time-dependent Schrödinger equation. Our work demonstrates that coincidence spectroscopy of ions and electrons is a powerful method for studying fundamental concepts of quantum information science within the context of ultrafast light-matter interactions.
The ion momentum distribution in the x-ray-induced dissociative photoionization of molecules is investigated, treating the ionization analytically under the Born-Oppenheimer approximation and simulating numerically the ion motion via the Schrödinger equation. The ion-photoelectron entanglement transfers information of the electronic interference to the ion dynamics. As a consequence, the ion momentum distributions of dissociative molecular photoionization present Young's double-slit interference when the photoelectron emission angle is fixed. We demonstrate that double-slit interference signatures persist in the ion longitudinal momentum shift even when the information of the correlated photoelectron is lost, which is the case for heteronuclear molecules when an additional photoelectron recoil momentum arises due to the different ion masses. For the case of sequential double ionization, we show that double-slit interference in the ion dynamics can be utilized for coherent control of the molecular dynamics.
We study the control of ionization dynamics of aligned N2{\mathrm{N}}_{2}N2​ and O2{\mathrm{O}}_{2}O2​ molecules in orthogonally polarized two-color (OTC) fields and calculate the photoelectron momentum distributions of molecules by solving the time-dependent Schr\"odinger equation and with a semiclassical model. In contrast with that of atoms in the OTC field, we show that the photoelectron momentum distribution is essentially dependent on the molecular outmost orbital, the alignment angle, and the phase of the OTC field. We illustrate the controlling of the molecular frame photoelectron angular distributions and the temporal and spatial double-slit interference effect for strong-field ionization of N2{\mathrm{N}}_{2}N2​ molecules. For O2{\mathrm{O}}_{2}O2​ molecules, it is shown that the ionization wave packets are splitting. The temporal and spatial double-slit interference effect is always present for O2{\mathrm{O}}_{2}O2​, which is not able to be turned off using the OTC field. This work would have implications for probing molecular structures with a two-color synthesized laser field.
A single-atom "double-slit" experiment is realized by photoionizing rubidium atoms using two independent low power lasers. The photoelectron wave of well-defined energy recedes to the continuum either from the 5P or 6P states in the same atom, resulting in two-path interference imaged in the far field using a photoelectron detector. Even though the lasers are independent and not phase locked, the transitions within the atom impart the phase relationship necessary for interference. The experiment is designed so that either 5P or 6P states are excited by one laser, before ionization by the second beam. The measurement cannot determine which excitation path is taken, resulting in interference in wave-vector space analogous to Young's double-slit studies. As the lasers are tunable in both frequency and intensity, the individual excitation-ionization pathways can be varied, allowing dynamic control of the interference term. Since the electron wave recedes in the Coulomb potential of the residual ion, a quantum model is used to capture the dynamics. Excellent agreement is found between theory and experiment.
We study a temporal version of Young's interference experiment by attosecond soft-x-ray pulses. The photoelectron energy spectra by attosecond double pulses exhibit an interference pattern, since we have no information on which pulse has generated the electron. We can re-establish the ``which-way'' information and control the interference visibility by changing the electron's momentum with phase-stabilized laser pulses, by an amount depending on the time of ionization. Moreover, if we use a triple pulse, we can realize a situation where the electron passes through a single and a double slit simultaneously to the same direction and is observed by the same detector.