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Optica

Interference of two-photon transitions induced by XUV light

M. Žitnik, A. Mihelič, K. Bučar, Špela Krušič, Richard James Squibb, R. Feifel, Iyas Ismail, P. Lablanquie, J. Palaudoux, Oksana Plekan, Michele Di Fraia, Marcello Coreno, Michele Manfredda, Alberto Simoncig, Primož Rebernik Ribič, Filippo Sottocorona, E. Allaria, Kevin Charles Prince, C. Callegari, Francis Jean Penent

Published May 20, 2022• 8 citations
Publisher

Abstract

The relative phase of first ( ω 1 ) and third harmonics ( ω 3 ) extreme ultraviolet light pulses was varied to control the population of the 2 s 2 state in helium through the interference of ω 1 + ω 1 and ω 3 − ω 1 two-photon excitation paths. The population was monitored by observing the total electron yield due to the 2 s 2 autoionization decay. Maximum yield occurs when the relative phase of the two harmonics matches the phase difference of complex atomic amplitudes governing the two excitation paths. The calculated trend of atomic phase differences agrees well with the measured data in the spectral region of the resonance, provided that time-reversed − ω 1 + ω 3 path is also taken into account. These results open the way to accessing phase differences of two-photon ionization paths involving energetically distant intermediate states and to perform interferometry in the extreme ultraviolet range by monitoring final state populations.

DOI
10.1364/optica.447436

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The relative phase of first ( ω 1 ) and third harmonics ( ω 3 ) extreme ultraviolet light pulses was varied to control the population of the 2 s 2 state in helium through the interference of ω 1 + ω 1 and ω 3 − ω 1 two-photon excitation paths. The population was monitored by observing the total electron yield due to the 2 s 2 autoionization decay. Maximum yield occurs when the relative phase of the two harmonics matches the phase difference of complex atomic amplitudes governing the two excitation paths. The calculated trend of atomic phase differences agrees well with the measured data in the spectral region of the resonance, provided that time-reversed − ω 1 + ω 3 path is also taken into account. These results open the way to accessing phase differences of two-photon ionization paths involving energetically distant intermediate states and to perform interferometry in the extreme ultraviolet range by monitoring final state populations.
Abstract Coherent control uses interference between quantum pathways to enhance or suppress transitions to a target quantum state. In stimulated Raman excitation, such control can be achieved through interference between two indistinguishable pathways connecting the same initial and final states, with the relative phase between the pathways modulating the population transfer to the final state. Extending this strategy to the extreme ultraviolet (XUV) and X-ray regimes would enable control of ultrafast electronic dynamics and site-selective core excitations. However, Raman coupling at short wavelengths competes with photoionization and intermediate-state decay, whereas intense fields with stable and adjustable relative phases remain difficult to produce. Here we use two-colour pulses from a seeded coherent free-electron laser to excite helium from its ground state to a bound metastable state via stimulated XUV Raman excitation. We implement phase-coherent control by creating two interfering Raman pathways through the ionization continuum and modulate the transferred population by varying their relative phases. Blocking one pathway removes the modulation, confirming its interferometric origin, and time-dependent Schrödinger equation calculations reproduce the measured phase dependence. Our results establish phase-controlled stimulated Raman excitation in the XUV regime, providing a strategy for the coherent control of atomic and molecular processes at short wavelengths.
Helium atoms in the presence of extreme ultraviolet light pulses can lose electrons through direct photoionization or through two-electron excitation followed by autoionization. Here we demonstrate that, by combining attosecond extreme ultraviolet pulses with near infrared femtosecond lasers, electron dynamics in helium autoionization can be not only monitored but also controlled. Furthermore, the interference between the two ionization channels was modified by the intense near infrared laser pulse. To the best of our knowledge, this is the first time that double excitation and autoionization were studied experimentally by using isolated attosecond pulses.
Phase-shift differences and amplitude ratios of the outgoing sss and ddd continuum wave packets generated by two-photon ionization of helium atoms are determined from the photoelectron angular distributions obtained using velocity map imaging. Helium atoms are ionized with ultrashort extreme-ultraviolet free-electron laser pulses with a photon energy of 20.3, 21.3, 23.0, and 24.3 eV, produced by the SPring-8 Compact SASE Source test accelerator. The measured values of the phase-shift differences are distinct from scattering phase-shift differences when the photon energy is tuned to an excited level or Rydberg manifold. The difference stems from the competition between resonant and non-resonant paths in two-photon ionization by ultrashort pulses. Since the competition can be controlled in principle by the pulse shape, the present results illustrate a new way to tailor the continuum wave packet.
Atoms irradiated with combined femtosecond laser and extreme ultraviolet (XUV) fields ionize through multiphoton processes, even when the energy of the XUV photon is below the ionization potential. However, in the presence of two different XUV photons and an intense laser field, it is possible to induce full electromagnetic transparency. Taking helium as an example, the laser field modifies its electronic structure, while the presence of two different XUV photons and the laser field leads to two distinct ionization pathways that can interfere destructively. This work demonstrates a new approach for coherent control in a regime of highly excited states and strong optical fields.
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.
We present a time- and phase-resolved, background-free scheme to study the extreme ultraviolet dipole emission of a bound electronic wave packet, without the use of any extreme ultraviolet exciting pulse. Using multiphoton transitions, we populate a superposition of quantum states which coherently emit extreme ultraviolet radiation through free induction decay. This emission is probed and controlled, both in amplitude and phase, by a time-delayed infrared femtosecond pulse. We directly measure the laser-induced dephasing of the emission by using a simple heterodyne detection scheme based on two-source interferometry. This technique provides rich information about the interplay between the laser field and the Coulombic potential on the excited electron dynamics. Its background-free nature enables us to use a large range of gas pressures and to reveal the influence of collisions in the relaxation process.