Modulation of attosecond beating in resonant two-photon ionization

We present a theoretical study of the photoelectron attosecond beating at the basis of RABBIT (Reconstruction of Attosecond Beating By Interference of Two-photon transitions) in the presence of autoionizing states. We show that, as a harmonic traverses a resonance, its sidebands exhibit a peaked phase shift as well as a modulation of the beating frequency itself. Furthermore, the beating between two resonant paths persists even when the pump and the probe pulses do not overlap, thus providing a sensitive non-holographic interferometric means to reconstruct coherent metastable wave packets. We characterize these phenomena quantitatively with a general finite-pulse analytical model that accounts for the effect of both intermediate and final resonances on two-photon processes, at a negligible computational cost. The model predictions are in excellent agreement with those of accurate ab initio calculations for the helium atom in the region of the N=2 doubly excited states

The Multi-Configurational Hartree-Fock close-coupling ansatz: application to Argon photoionization cross section and delays

We present a robust, ab initio method for addressing atom-light interactions and apply it to photoionization of argon. We use a close-coupling ansatz constructed on a multi-configurational Hartree-Fock description of localized states and B-spline expansions of the electron radial wave functions. In this implementation, the general many-electron problem can be tackled thanks to the use of the ATSP2K libraries [CPC 176 (2007) 559]. In the present contribution, we combine this method with exterior complex scaling, thereby allowing for the computation of the complex partial amplitudes that encode the whole dynamics of the photoionization process. The method is validated on the 3s3p6np series of resonances converging to the 3s extraction. Then, it is used for computing the energy dependent differential atomic delay between 3p and 3s photoemission, and agreement is found with the measurements of Gu\'enot et al. [PRA 85 (2012) 053424]. The effect of the presence of resonances in the one-photon spectrum on photoionization delay measurements is studied.Comment: 15 pages, 8 figures, 4 table

Molecular-frame photoelectron angular distributions of CO in the vicinity of feshbach resonances: an xchem approach

The advent of ultrashort XUV pulses is pushing for the development of accurate theoretical calculations to describe ionization of molecules in regions where electron correlation plays a significant role. Here, we present an extension of the XCHEM methodology to evaluate laboratory- and molecular-frame photoelectron angular distributions in the region where Feshbach resonances are expected to appear. The performance of the method is demonstrated in the CO molecule, for which information on Feshbach resonances is very scarce. We show that photoelectron angular distributions are dramatically affected by the presence of resonances, to the point that they can completely reverse the preferred electron emission direction observed in direct nonresonant photoionization. This is the consequence of significant changes in the electronic structure of the molecule when resonances decay, an effect that is mostly driven by electron correlation in the ionization continuum. The present methodology can thus be helpful for the interpretation of angularly resolved photoionization time delays in this and more complex moleculesThe work was supported by the European COST Action AttoChem (CA18222) and the Spanish State Research Agency (AEI/ 10.13039/501100011033), Grants PID2019-105458RB-I00 and PID2019-106732GB-I00, “Severo Ochoa” Programme for Centres of Excellence in R&D (SEV-2016-0686) and “María de Maeztu” Programme for Units of Excellence in R&D (CEX2018-000805-M

Attosecond photoionization delays in the vicinity of molecular Feshbach resonances

Temporal delays extracted from photoionization phases are currently determined with attosecond resolution by using interferometric methods. Such methods require special care when photoionization occurs near Feshbach resonances due to the interference between direct ionization and autoionization. Although theory can accurately handle these interferences in atoms, in molecules, it has to face an additional, so far insurmountable problem: Autoionization is slow, and nuclei move substantially while it happens, i.e., electronic and nuclear motions are coupled. Here, we present a theoretical framework to account for this effect and apply it to evaluate time-resolved and vibrationally resolved photoelectron spectra and photoionization phases of N2 irradiated by a combination of an extreme ultraviolet (XUV) attosecond pulse train and an infrared pulse. We show that Feshbach resonances lead to unusual non-Franck-Condon vibrational progressions and to ionization phases that strongly vary with photoelectron energy irrespective of the vibrational state of the remaining molecular cationThis work was supported by European COST Action CA18222 AttoChem; the Synergy Grant of the European Research Council TOMATTO (ref. 951224); the projects PDC2021-121073-I00, PID2019-105458RB-I00, and PID2019-106732GB-I00 funded by MCIN/AEI /10.13039/501100011033 and by the European Union “NextGenerationEU”/PRTRMICINN programs; the Comunidad de Madrid project FULMATEN (ref. Y2018NMT-5028); the “Severo Ochoa” Programme for Centres of Excellence in R&D (CEX2020-001039-S); and the “Maria de Maeztu” Programme for Units of Excellence in R&D (CEX2018-000805-M). L.A. acknowledges the DOE CAREER grant no. DE-SC0020311V and the NSF grant PHY-1912507. V.J.B. thanks the MICINN for the FPI grant (BES-2017-081521) related to the project FIS2016-77889-

Attosecond electron spectroscopy using a novel interferometric pump-probe technique

We present an interferometric pump-probe technique for the characterization of attosecond electron wave packets (WPs) that uses a free WP as a reference to measure a bound WP. We demonstrate our method by exciting helium atoms using an attosecond pulse with a bandwidth centered near the ionization threshold, thus creating both a bound and a free WP simultaneously. After a variable delay, the bound WP is ionized by a few-cycle infrared laser precisely synchronized to the original attosecond pulse. By measuring the delay-dependent photoelectron spectrum we obtain an interferogram that contains both quantum beats as well as multi-path interference. Analysis of the interferogram allows us to determine the bound WP components with a spectral resolution much better than the inverse of the attosecond pulse duration.Comment: 5 pages, 4 figure

Uncertainties in Theoretical HeI Emissivities: HII Regions, Primordial Abundance, and Cosmological Recombination

A number of recent works in astronomy and cosmology have relied upon theoretical He I emissivities, but we know of no effort to quantify the uncertainties in the atomic data. We analyze and assign uncertainties to all relevant atomic data, perform Monte Carlo analyses, and report standard deviations in the line emissivities. We consider two sets of errors, which we call "optimistic" and "pessimistic." We also consider three different conditions, corresponding to prototypical Galactic and extragalactic H II regions and the epoch of cosmological recombination. In the extragalactic H II case, the errors we obtain are comparable to or larger than the errors in some recent $Y_p$ calculations, including those derived from CMB observations. We demonstrate a systematic effect on primordial abundance calculations; this effect cannot be reduced by observing a large number of objects. In the cosmological recombination case, the errors are comparable to many of the effects considered in recent calculations.Comment: 5 pages, 3 figures, accepted to MNRAS Letter

Reconstruction and control of a time-dependent two-electron wave packet

The concerted motion of two or more bound electrons governs atomic1 and molecular2,3 non-equilibrium processes including chemical reactions, and hence there is much interest in developing a detailed understanding of such electron dynamics in the quantum regime. However, there is no exact solution for the quantumthree-body problem, and as a result even the minimal system of two active electrons and a nucleus is analytically intractable4. This makes experimental measurements of the dynamics of two bound and correlated electrons, as found in the helium atom, an attractive prospect.However, although the motion of single active electrons and holes has been observed with attosecond time resolution5-7, comparable experiments on two-electron motion have so far remained out of reach. Here we showthat a correlated two-electron wave packet can be reconstructed froma 1.2-femtosecondquantumbeatamong low-lying doubly excited states in helium.The beat appears in attosecond transient-absorption spectra5,7-9 measured with unprecedentedly high spectral resolution and in the presence of an intensity-tunable visible laser field.Wetune the coupling10-12 between the two low-lying quantum states by adjusting the visible laser intensity, and use the Fano resonance as a phase-sensitive quantum interferometer13 to achieve coherent control of the two correlated electrons. Given the excellent agreement with large-scalequantum-mechanical calculations for thehelium atom, we anticipate thatmultidimensional spectroscopy experiments of the type we report here will provide benchmark data for testing fundamental few-body quantumdynamics theory in more complex systems. Theymight also provide a route to the site-specificmeasurement and control of metastable electronic transition states that are at the heart of fundamental chemical reactionsWe thank E. Lindroth for calculating the dipole moment (2p2|r|sp2,3+), and also A. Voitkiv, Z.-H. Loh, and R. Moshammer for helpful discussions. We acknowledge financial support by the Max-Planck Research Group Program of the Max-Planck Gesellschaft (MPG) and the European COST Action CM1204 XLIC. L. A. and F. M. acknowledge computer time from the CCC-UAM and Mare Nostrum supercomputer centers and financial support by the European Research Council under the ERC Advanced Grant no. 290853 XCHEM, the Ministerio de Economía y Competitividad projects FIS2010-15127, FIS2013-42002-R and ERA-Chemistry PIM2010EEC-00751, and the European grant MC-ITN CORIN

Attosecond dynamics through a Fano resonance: Monitoring the birth of a photoelectron

This is the author’s version of the work. It is posted here by permission of the AAAS for personal use, not for redistribution. The definitive version was published in Science on 354, 11 november 2016, DOI: 10.1126/science.aah5188The dynamics of quantum systems are encoded in the amplitude and phase of wave packets. However, the rapidity of electron dynamics on the attosecond scale has precluded the complete characterization of electron wave packets in the time domain. Using spectrally resolved electron interferometry, we were able to measure the amplitude and phase of a photoelectron wave packet created through a Fano autoionizing resonance in helium. In our setup, replicas obtained by two-photon transitions interfere with reference wave packets that are formed through smooth continua, allowing the full temporal reconstruction, purely from experimental data, of the resonant wave packet released in the continuum. In turn, this resolves the buildup of the autoionizing resonance on an attosecond time scale. Our results, in excellent agreement with ab initio time-dependent calculations, raise prospects for detailed investigations of ultrafast photoemission dynamics governed by electron correlation, as well as coherent control over structured electron wave packetsWe thank S. Weber for crucial contributions to the PLFA attosecond beamline, D. Cubaynes, M. Meyer, F. Penent, J. Palaudoux, for setup and test of the electron spectrometer, and O. Smirnova, for fruitful discussions. Supported by ITN-MEDEA 641789, ANR-15-CE30-0001-01-CIMBAAD, ANR11-EQPX0005-ATTOLAB, the European Research Council Advanced Grant XCHEM no. 290853, the European COST Action XLIC CM1204, and the MINECO Project no. FIS2013-42002-R. We acknowledge allocation of computer time from CCC-UAM and Mare Nostrum BS

Caracterização do perfil sorológico de nulíparas suínas e da progênie frente ao parvovírus suíno.

Projeto: 03.09.00.046