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arXiv:1807.11762 · Physical Review Letters

Coherent Control of Penning and Associative Ionization: Insights from Symmetries

Juan J. Omiste, Johannes Floß, Paul W. Brumer

Published Oct 17, 2018• 14 citations
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Abstract

Coherent control of reactive atomic and molecular collision processes remains elusive experimentally due to quantum interference-based requirements. Here, with insights from symmetry conditions, a viable method for controlling Penning and associative ionization in atomic collisions is proposed. Computational applications to He^{*}(^{3}S)-Li(^{2}S) and Ne^{*}(^{3}P_{2})-Ar(^{1}S_{0}) show extensive control over the ionization processes under experimentally feasible conditions.

DOI
10.1103/physrevlett.121.163405

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Coherent control of reactive atomic and molecular collision processes remains elusive experimentally due to quantum interference-based requirements. Here, with insights from symmetry conditions, a viable method for controlling Penning and associative ionization in atomic collisions is proposed. Computational applications to He^{}(^{3}S)-Li(^{2}S) and Ne^{}(^{3}P_{2})-Ar(^{1}S_{0}) show extensive control over the ionization processes under experimentally feasible conditions.
Coherent control theory is applied to the control of Ne*(3s,(3)P2)+Ar((1)S0) collisions and computations are shown that display extensive control over these processes. Indeed we demonstrate that it is possible to essentially turn on and off the cross sections for both the Penning and associative ionization processes. This facility arises from the interference between matter waves induced by creating a linear superposition of the degenerate M={-2,-1,0,1,2} Zeeman sublevels of the Ne*(3s,(3)P2) target atom. The computations, conducted at collision energies in the 1-8 kcal/mole range, are based on combining, within the "rotating atom approximation," empirically derived and ab initio ionization widths.
We explore coherent control of Penning and associative ionization in cold collisions of metastable He∗(23S){\mathrm{He}}^{*}(2{\phantom{\rule{4pt}{0ex}}}^{3}S)He∗(23S) atoms via the quantum interference between different states of the He2∗{\mathrm{He}}_{2}^{*}He2∗​ collision complex. By tuning the preparation coefficients of the initial atomic spin states, we can benefit from the quantum interference between molecular channels to maximize or minimize the cross sections for Penning and associative ionization. In particular, we find that we can enhance the ionization ratio by 30% in the cold regime. This work is significant for the coherent control of chemical reactions in the cold and ultracold regimes.
Coherent control techniques are computationally applied to cold (1  mK<T<1  K1\text{ }\text{ }\mathrm{mK}<T<1\text{ }\text{ }\mathrm{K}1  mK<T<1  K) and ultracold ($T<1\text{ }\text{ }\ensuremath{\mu}\mathrm{K}$) Ne∗(3s,3P2)+Ar(1S0){\mathrm{Ne}}^{*}(3s,^{3}P_{2})+\mathrm{Ar}(^{1}S_{0})Ne∗(3s,3P2​)+Ar(1S0​) collisions. We show that by using various initial superpositions of the Ne∗(3s,3P2){\mathrm{Ne}}^{*}(3s,^{3}P_{2})Ne∗(3s,3P2​) $M={\ensuremath{-}2,\ensuremath{-}1,0,1,2}$ Zeeman sublevels it is possible to reduce the Penning ionization and associative ionization cross sections by as much as 4 orders of magnitude. It is also possible to drastically change the ratio of these two processes. The results are based on combining, within the ``rotating atom approximation'', empirical and ab initio ionization widths.
Quantitative control and measurement of quantum entanglement are essential for advancing quantum technologies. Photoionization induced by ultrashort laser pulses provides a unique platform for studying entanglement between photoelectrons and residual ions, representing one of the most intriguing quantum phenomena in attosecond physics. Although extensive studies have focused on the coherence properties within either the emitted electrons or the ions individually, the electron-ion entanglement has remained largely unexplored. In this work, we bridge this gap by investigating the resonance-enhanced multiphoton ionization of argon atoms driven by two time-delayed ultrashort ultraviolet pulses. Employing state-of-the-art first-principles multi-electron simulations, we demonstrate the ability to reconstruct and precisely manipulate the purity of electron quantum states through detailed analysis of the photoelectron angular distributions. Our results reveal distinct scattering-phase differences among various electron configurations within the same partial wave channel, providing unequivocal evidence of electron-ion correlation and entanglement. With the fast development of free-electron lasers, this study establishes an experimentally feasible framework for directly controlling quantum entanglement in ultrafast ionization processes, offering new insights and powerful methodologies for exploring complex electron dynamics in many-electron systems.
The subtle and fundamental issue of indistinguishability and interference between independent pathways to the same target state is examined in the context of coherent control of atomic and molecular processes, with emphasis placed on possible "which-way" information due to quantum entanglement established in the quantum dynamics. Because quantum interference between independent pathways to the same target state occurs only when the independent pathways are indistinguishable, it is first shown that creating useful coherence between nondegenerate states of a molecule for subsequent quantum interference manipulation cannot be achieved by collisions between atoms or molecules that are prepared in momentum and energy eigenstates. Coherence can, however, be transferred from light fields to atoms or molecules. Using a particular coherent control scenario, it is shown that this coherence transfer and the subsequent coherent phase control can be readily realized by the most classical states of light, i.e., coherent states of light. It is further demonstrated that quantum states of light may suppress the extent of phase-sensitive coherent control by leaking out some which-way information while "incoherent interference control" scenarios proposed in the literature have automatically ensured the indistinguishability of multiple excitation pathways. The possibility of quantum coherence in photodissociation product states is also understood in terms of the disentanglement between photodissociation fragments. Results offer deeper insights into quantum coherence generation in atomic and molecular processes.
Coherent control provides a quantum interference based method for controlling atomic and molecular dynamics. We report two experimental observations of different ways to achieve such a control in atomic photoionization continuum. One is the photoionization of sodium atoms, initially prepared in the 3P1/2 excited state, by a non resonant three-photon interaction with 1064-nm laser light and by a one-photon interaction with the third-harmonic field, at 355 nm. Interference between the two transition paths allows the control of the total ionization rate by varying the relative phase of the laser fields. The second experiment is the observation of the modification of the ionization continua of xenon through laser induced continuum structure (LICS). The multiphoton radiative decay of the xenon ground state into the two electronic continua, that correspond to the two fine structure levels of the ground state of the xenon ion, is varied by electromagnetically embedding a bound state of the atom into the two continua. Both experiments are performed on an atomic beam apparatus which uses a time-of-flight spectrometer for energy analyzing the emitted photoelectrons.