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Physical Review A

Attosecond electron interferometry for measurement of the quantum phase of free-electron wave packets

Candong Liu, M. Nisoli

Published Nov 5, 2012• 5 citations
Publisher

Abstract

Single-photon ionization of a hydrogen atom irradiated by two time-delayed isolated attosecond pulses is theoretically investigated by numerically solving the fully three-dimensional time-dependent Schr\"odinger equation. It is demonstrated that the analysis of the angular-resolved electron energy spectrum, showing a complex interference pattern, allows one to completely retrieve the difference between the energy-dependent phases of the electron wave packets generated by the two delayed attosecond pulses. Moreover, it is shown that in the case of a pair of excitation pulses with the same chirp rate, the proposed interferometric technique can be used to measure the difference between the carrier envelope phase values of two attosecond pulses.

DOI
10.1103/physreva.86.053404

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To time-resolve attosecond electronic dynamics in general photoionization processes, the technique that retrieves the phase of emitted electronic wave packets without intercepting the interactions is essential. Here, we theoretically demonstrate a scheme that uses isolated attosecond pulses (IAPs) to achieve this goal. Our approach utilizes the coherent interference between the electronic wave packets of interest and the one produced by a subsequent IAP. It is shown that the photoelectron spectral phase that has eluded direct detection so far can be fully recovered from observable photoelectron spectra without perturbing the electron-release process under investigation. By further performing a time-frequency-like analysis on the photoelectron energy spectra with the spectral phase, we reveal the birth processes of photoelectrons in time and the association between electronic energy and birth time in strong-field ionization driven by circularly polarized laser pulses. The present work explores a promising application of IAPs for ultrafast measurement and opens a viable venue for investigating electronic dynamics with quantum phase information.

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Physical Review Letters•Oct 15, 2024•31 citations
Single-photon ionization of a hydrogen atom irradiated by two time-delayed isolated attosecond pulses is theoretically investigated by numerically solving the fully three-dimensional time-dependent Schr"odinger equation. It is demonstrated that the analysis of the angular-resolved electron energy spectrum, showing a complex interference pattern, allows one to completely retrieve the difference between the energy-dependent phases of the electron wave packets generated by the two delayed attosecond pulses. Moreover, it is shown that in the case of a pair of excitation pulses with the same chirp rate, the proposed interferometric technique can be used to measure the difference between the carrier envelope phase values of two attosecond pulses.
To time-resolve attosecond electronic dynamics in general photoionization processes, the technique that retrieves the phase of emitted electronic wave packets without intercepting the interactions is essential. Here, we theoretically demonstrate a scheme that uses isolated attosecond pulses (IAPs) to achieve this goal. Our approach utilizes the coherent interference between the electronic wave packets of interest and the one produced by a subsequent IAP. It is shown that the photoelectron spectral phase that has eluded direct detection so far can be fully recovered from observable photoelectron spectra without perturbing the electron-release process under investigation. By further performing a time-frequency-like analysis on the photoelectron energy spectra with the spectral phase, we reveal the birth processes of photoelectrons in time and the association between electronic energy and birth time in strong-field ionization driven by circularly polarized laser pulses. The present work explores a promising application of IAPs for ultrafast measurement and opens a viable venue for investigating electronic dynamics with quantum phase information.
Within this work, electron dynamics in atoms are experimentally and numerically investigated on their natural attosecond time scales. To access these dynamics, ultrashort and moderately-intense few-cycle laser pulses are superposed with attosecond pulsed radiation in the extreme-ultraviolet spectral region. Both these sources are combined in a new experimental vacuum setup which was designed and built up from scratch, also in order to generate the attosecond pulses. Novel experimental schemes are developed which involve the temporal and spectral interferometric utilization of both ultrashort light sources and include the multidimensional spectroscopy employing different dynamical parameters. These are the intensity and the carrier-envelope phase of the laser pulses, as well as their temporal delay with respect to the attosecond pulses. Scientifically, the observation and control of the quantum-motion of bound electrons, as well as the laser-driven quasi-classical motion of free electrons was a key goal of this work. In particular, a bound two-electron wave packet in helium on attosecond time scales was experimentally observed for the first time. This was realized by combining unprecedented high temporal and spectral resolution. In addition, a new coupling mechanism of several doubly-excited states to an effective single-electron continuum is identified and analyzed. Both these two-electron states as well as single-electron states are interferometrically investigated with access to the phase of their quantum-mechanical wave function. This allows the observation and control of the quantum dynamics of two correlated electrons in atoms on the attosecond time scale which was demonstrated within the scope of this work.
Ultrafast atomic processes, such as excitation and ionization occurring on the femtosecond or shorter time scale, were explored by employing attosecond high-harmonic pulses. With the absorption of a suitable high-harmonic photon a He atom was ionized, or resonantly excited with further ionization by absorbing a number of infrared photons. The electron wave packets liberated by the two processes generated an interference containing the information on ultrafast atomic dynamics. The attosecond electron wave packet, including the phase, from the ground state was reconstructed first and, subsequently, that from the 1s3p state was retrieved by applying the holographic technique to the photoelectron spectra comprising the interference between the two ionization paths. The reconstructed electron wave packet revealed details of the ultrafast photoionization dynamics, such as the instantaneous two-photon ionization rate.
The age of attosecond physics was ushered in by the invention of methods for probing phenomena on a time scale less than femtoseconds [F. Krausz, M. Ivanov, Rev. Mod. Phys. 81, 163 (2009)]. In photoemission, the Eisenbud-Wigner-Smith (EWS) time delay [R. Pazourek, S. Nagele, J. Burgdorfer, Rev. Mod. Phys. 87, 765 (2015)] is the interval between photon annihilation and emission of the electron, usually measured in attoseconds (10−1810^{-18}10−18 seconds), and varies with the kinetic energy and the angle of emission of the electron wave packet. We present a new interferometric method of measurement, using two phase-locked Extreme Ultraviolet pulses of frequency ω\omegaω and 2ω2\omega2ω, from a Free-Electron Laser. Phase differences between one- and two-photon ionization channels are extracted, and used to derive the relative EWS delay for one- and two-photon ionization of neon as a function of emission angle. Agreement with theory is excellent. Competing techniques require the use of an IR field, which necessitates corrections, but our method is correction-free. This new quantum clock is a powerful tool for investigating ultrafast processes in atoms and molecules.
Summary form only given. Angstrom and attosecond control of free electron wave packets is one of the pinnacles of attosecond science. Orthogonally polarized two-color (OTC) laser fields allow to control the motion of field-ionizing electronic wave packets both in time and space[1]. In OTC pulses time and space are connected and thus an attosecond time scale is established in the polarization plane for both the emitted and the re-colliding wave packets[2,3].In this submission, we report on experiments that use OTC pulses for studying atomic single and double ionization. The three-dimensional momentum vector of electrons and ions created by single and double ionization of neon atoms was measured with the COLTRIMS technique as a function of the sub-cycle shape of the OTC pulses. We introduce a concept similar to attosecond streaking that allows reading sub-cycle timing information from the momentum vector of emitted electrons. The concept is then applied to gaining information about the influence of the long-range Coulomb potential on the trajectories of tunneling electrons.Fig.1 (a) shows the measured momentum distributions of electrons correlated with singly ionized neon in the polarization plane of the OTC field with relative phase Δφ between the two color components. The spectra show that the electron emission direction is sensitive to Δφ. Furthermore, the spectra feature a prominent x-shaped central structure and weaker fine-scale modulations due to wave packet interferences. To compare with simulated spectra with strong field approximation (SFA) and solving two-dimensional time-dependent Schrödinger equation (TDSE) with single active electron approximation, we conclude that Coulomb effect plays important role on the spatial distribution of released electron wave packets. In the conference, we will furthermore demonstrate control over the correlation between the two electrons emitted during double ionization upon electron recollision by tuning the shape of the electric field of the OTC pulses on the sub-cycle scale. The results of these experiments are in agreement with theoretical predictions [4].
Attosecond chronoscopy enables the exploration of correlated electron dynamics in real time. One key observable of attosecond physics is the determination of "time zero" of photoionization, the time delay with which the wave packet of the ionized electron departs from the ionic core. This observable has become accessible by experimental advances in attosecond streaking and reconstruction of attosecond beating by interference of two-photon transitions (RABBIT) techniques. In this Letter, we explore photoionization time delays by strong extreme ultraviolet fields beyond the linear-response limit. We identify novel signatures in time delays signifying strong coupling between atoms and light fields and the light-field dressing of the ion. As a prototypical case, we study the interelectronic coherence and entanglement in helium driven by a strong extreme ultraviolet field. By the numerical solution of the time-dependent Schrödinger equation in its full dimensionality, we show that the time delay of the photoionized electron allows one to monitor the ultrafast variations of coherence dynamics and entanglement in real time.