Complete Photoionization Experiments via Ultrafast Coherent Control with Polarization Multiplexing

Hockett, Paul; Wollenhaupt, M.; Lux, Christian; Baumert, Thomas

doi:10.1103/physrevlett.112.223001

Cited by 46 publications

(79 citation statements)

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“…In these studies, scattering phases were only determined at a single energy. Based on this work, the first "complete" photoionization measurements [29][30][31] provided access to the phases and amplitudes of the ionization matrix element. Here we report on the angular dependence of the photoionization process in the time domain by probing the electron with a phase-locked laser field at several different photoelectron energies using RABBITT.…”

Section: Introductionmentioning

confidence: 99%

Angular dependence of photoemission time delay in helium

et al. 2016

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Time delays of electrons emitted from an isotropic initial state with the absorption of a single photon and leaving behind an isotropic ion are angle independent. Using an interferometric method involving XUV attosecond pulse trains and an IR-probe field in combination with a detection scheme, which allows for full three-dimensional momentum resolution, we show that measured time delays between electrons liberated from the 1s 2 spherically symmetric ground state of helium depend on the emission direction of the electrons relative to the common linear polarization axis of the ionizing XUV light and the IR-probing field. Such time delay anisotropy, for which we measure values as large as 60 as, is caused by the interplay between final quantum states with different symmetry and arises naturally whenever the photoionization process involves the exchange of more than one photon. With the support of accurate theoretical models, the angular dependence of the time delay is attributed to small phase differences that are induced in the laser-driven continuum transitions to the final states. Since most measurement techniques tracing attosecond electron dynamics involve the exchange of at least two photons, this is a general and significant effect that must be taken into account in all measurements of time delays involving photoionization processes.

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Section: Introductionmentioning

confidence: 99%

Angular dependence of photoemission time delay in helium

et al. 2016

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“…As described above, in this work we are concerned with the additional insight available from 3D measurements, so the reader is referred to Refs. [21,29] for full details of the ionization process, including the ionization pathways, angular momentum coupling diagrams, and the full theoretical treatment.…”

Section: Photoelectron Metrologymentioning

confidence: 99%

“…For example, photoelectron interferograms have been used to obtain complete information on the scattering wave function for both atoms and molecules [6][7][8][9][10]; to investigate electron correlation and entanglement in multiple ionization [3,11]; and in the related context of photoelectron diffraction [12] and photoelectron holography [13,14], wherein intense laser fields are used to drive rescattering of continuum waves from the photoion and, in the case of holography, additional interferences between direct (reference) and the rescattered continuum waves are observed. Furthermore, in time-dependent cases, the continuum wave function will respond to the underlying dynamics of the ionizing system, for instance evolving electronic or nuclear configurations [15][16][17][18][19], which may in turn depend on the properties of the laser pulse(s) applied and even allow for control [20,21]. It is also of note that the scattering phase accumulated by the partial waves is correlated, in the time domain, with the relative ionization time delay, often termed the Wigner delay [22,23].…”

Section: Introductionmentioning

confidence: 99%

“…While it is trivial to state that 3D measurements offer a higher information content than 2D measurements, the restrictions inherent to 2D measurements are highly detrimental to the understanding of the photoelectron interference pattern and the concomitant ability to use subtle changes in this pattern as a probe of the underlying quantum mechanics. This statement becomes more applicable as the complexity of the light-matter interaction grows and the number of interfering pathways increases; for instance, ionization with polarizationshaped laser pulses, where highly structured, noncylindrically symmetric, photoelectron distributions are the norm [20,21]. Figure 1 illustrates some of these concepts in photoelectron interferometry and imaging, with an example angular interferogram I (θ,φ), representations in velocity space for [ Fig.…”

Section: Introductionmentioning

confidence: 99%

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Maximum-information photoelectron metrology

et al. 2015

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Access and use of this website and the material on it are subject to the Terms and Conditions set forth at Maximum-information photoelectron metrology Hockett, P.; Lux, C.; Wollenhaupt, M.; Baumert, T.http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/jsp/nparc_cp.jsp?lang=fr L'accès à ce site Web et l'utilisation de son contenu sont assujettis aux conditions présentées dans le site LISEZ CES CONDITIONS ATTENTIVEMENT AVANT D'UTILISER CE SITE WEB. NRC Publications Record / Notice d'Archives des publications de CNRC:http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/ctrl?action=rtdoc&an=21276916&lang=en http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/ctrl?action=rtdoc&an=21276916&lang=fr READ THESE TERMS AND CONDITIONS CAREFULLY BEFORE USING THIS WEBSITE.http://nparc.cisti-icist.nrc-cnrc.gc.ca/npsi/jsp/nparc_cp.jsp?lang=en Vous avez des questions? Nous pouvons vous aider. Pour communiquer directement avec un auteur, consultez la première page de la revue dans laquelle son article a été publié afin de trouver ses coordonnées. Si vous n'arrivez pas à les repérer, communiquez avec nous à PublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. Questions? Contact the NRC Publications Archive team atPublicationsArchive-ArchivesPublications@nrc-cnrc.gc.ca. If you wish to email the authors directly, please see the first page of the publication for their contact information. NRC Publications Archive Archives des publications du CNRCThis publication could be one of several versions: author's original, accepted manuscript or the publisher's version. / La version de cette publication peut être l'une des suivantes : la version prépublication de l'auteur, la version acceptée du manuscrit ou la version de l'éditeur. For the publisher's version, please access the DOI link below./ Pour consulter la version de l'éditeur, utilisez le lien DOI ci-dessous.http://doi.org/10.1103/PhysRevA.92.013412Physical Review A: Atomic, Molecular, and Optical Physics, 92, 1, 2015-07-13 Photoelectron interferograms, manifested in photoelectron angular distributions (PADs), are high-information, coherent observables. In order to obtain the maximum information from angle-resolved photoionization experiments it is desirable to record the full, three-dimensional (3D), photoelectron momentum distribution. Here we apply tomographic reconstruction techniques to obtain such 3D distributions from multiphoton ionization of potassium atoms, and fully analyze the energy and angular content of the 3D data. The PADs obtained as a function of energy indicate good agreement with previous 2D data and detailed analysis [Hockett et al., Phys. Rev. Lett. 112, 223001 (2014)] concerning the main spectral features, but also indicate unexpected symmetry breaking in certain regions of momentum space, thus revealing additional continuum interferences which cannot otherwise be observed. These observations reflect the presence of additional ionization pathways and, most generally, illustrate the power of maximum-information measurements of coherent observables for quantum metrology of c...

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“…In the energy domain, a number of different schemes have been demonstrated in both the laboratory (LF) and molecular frames (MF) [10][11][12][13][14][15][16]. The common theme to all these measurements is some form of control over the experimental contributions to the photoionization interferometer (e.g.…”

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confidence: 99%

Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry

et al. 2017

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Photoionization of molecular species is, essentially, a multi-path interferometer with both experimentally controllable and intrinsic molecular characteristics. In this work, XUV photoionization of impulsively aligned molecular targets (N2) is used to provide a time-domain route to "complete" photoionization experiments, in which the rotational wavepacket controls the geometric part of the photoionization interferometer. The data obtained is sufficient to determine the magnitudes and phases of the ionization matrix elements for all observed channels, and to reconstruct molecular frame interferograms from lab frame measurements. In principle this methodology provides a timedomain route to complete photoionization experiments, and the molecular frame, which is generally applicable to any molecule (no prerequisites), for all energies and ionization channels.Photoionization is an interferometric process, in which the final observable results from a coherent sum over multiple quantum paths to a set of final continuum photoelectron states |k, l, m [1,2]. Interferences between these components are manifest in the observable energy spectra and photoelectron angular distributions (PADs) [2][3][4], the latter of which can be considered as a particularly high information content observable, extremely sensitive to the phases of the partial waves |l, m [4, 5]; consequently, PADs have been investigated in a large range of control and metrology scenarios [6,7] . In the context of phase-sensitive metrology, the goal is to obtain the full set of complex photoionization matrix elements, hence characterise the photoelectron wavefunction, by analysis of sets of PAD measurements -this is a "complete" photoionization experiment [8,9].In the molecular case, the number of final |l, m states is typically large, and obtaining a sufficient dataset for a complete experiment remains a challenge. In the energy domain, a number of different schemes have been demonstrated in both the laboratory (LF) and molecular frames (MF) [10][11][12][13][14][15][16]. The common theme to all these measurements is some form of control over the experimental contributions to the photoionization interferometer (e.g. rotational state, polarization geometry), to which the intrinsic molecular contributions remain invariant. The difficulties in such cases are the ability to obtain a sufficiently large dataset, and molecular specificity in the methodologies, i.e. prerequisites such as low density of states [14], resonances [15] or dissociative channels [11][12][13].In the time-domain, rotational wavepackets can be utilized to control the geometric part of the interferometer. In this case, a high degree of spatio-temporal control of the axis distribution (alignment) of the ionizing molecular ensemble in the LF can be obtained via preparation of a broad rotational wavepacket. Although this idea is conceptually obvious, the theory is complex; it has been elucidated by multiple authors (e.g. refs. [5,[17][18][19][20][21]), but -to date -there have been no experimental d...

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Complete Photoionization Experiments via Ultrafast Coherent Control with Polarization Multiplexing

Cited by 46 publications

References 38 publications

Angular dependence of photoemission time delay in helium

Angular dependence of photoemission time delay in helium

Maximum-information photoelectron metrology

Molecular Frame Reconstruction Using Time-Domain Photoionization Interferometry

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