| 1. |
- Isinger, M., et al.
(författare)
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Photoionization in the time and frequency domain
- 2017
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Ingår i: Science. - : American Association for the Advancement of Science (AAAS). - 0036-8075 .- 1095-9203. ; 358:6365, s. 893-6
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Tidskriftsartikel (refereegranskat)abstract
- Ultrafast processes in matter, such as the electron emission following light absorption, can now be studied using ultrashort light pulses of attosecond duration (10−18 s) in the extreme ultraviolet spectral range. The lack of spectral resolution due to the use of short light pulses has raised issues in the interpretation of the experimental results and the comparison with theoretical calculations. We determine photoionization time delays in neon atoms over a 40 eV energy range with an interferometric technique combining high temporal and spectral resolution. We spectrally disentangle direct ionization from ionization with shake-up, in which a second electron is left in an excited state, and obtain excellent agreement with theoretical calculations, thereby solving a puzzle raised by 7-year-old measurements.
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| 2. |
- Petersson, C. L.M., et al.
(författare)
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Anisotropic photoemission time delays close to a Fano resonance
- 2018
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 9
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Tidskriftsartikel (refereegranskat)abstract
- Electron correlation and multielectron effects are fundamental interactions that govern many physical and chemical processes in atomic, molecular and solid state systems. The process of autoionization, induced by resonant excitation of electrons into discrete states present in the spectral continuum of atomic and molecular targets, is mediated by electron correlation. Here we investigate the attosecond photoemission dynamics in argon in the 20-40 eV spectral range, in the vicinity of the 3s(-1)np autoionizing resonances. We present measurements of the differential photoionization cross section and extract energy and angle-dependent atomic time delays with an attosecond interferometric method. With the support of a theoretical model, we are able to attribute a large part of the measured time delay anisotropy to the presence of autoionizing resonances, which not only distort the phase of the emitted photoelectron wave packet but also introduce an angular dependence.
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| 3. |
- Zhong, Shiyang, et al.
(författare)
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Attosecond electron–spin dynamics in Xe 4d photoionization
- 2020
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723 .- 2041-1723. ; 11:1
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Tidskriftsartikel (refereegranskat)abstract
- The photoionization of xenon atoms in the 70–100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe+ states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as, and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide insight into the complex electron-spin dynamics of photo-induced phenomena.
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| 4. |
- Brizuela, Fernando, et al.
(författare)
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Efficient high order harmonic generation boosted by below threshold harmonics
- 2013
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Ingår i: Scientific Reports. - : Springer Science and Business Media LLC. - 2045-2322. ; 3
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Tidskriftsartikel (refereegranskat)abstract
- High-order harmonic generation (HHG) in gases has been established as an important technique for the generation of coherent extreme ultraviolet (XUV) pulses at ultrashort time scales. Its main drawback, however, is the low conversion efficiency, setting limits for many applications, such as ultrafast coherent imaging, nonlinear processes in the XUV range, or seeded free electron lasers. Here we introduce a novel scheme based on using below-threshold harmonics, generated in a seeding cell, to boost the HHG process in a generation cell, placed further downstream in the focused laser beam. By modifying the fundamental driving field, these low-order harmonics alter the ionization step of the nonlinear HHG process. Our dual-cell scheme enhances the conversion efficiency of HHG, opening the path for the realization of robust intense attosecond XUV sources.
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| 5. |
- Carette, Thomas, et al.
(författare)
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Multiconfigurational Hartree-Fock close-coupling ansatz : Application to the argon photoionization cross section and delays
- 2013
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 87:2, s. 023420-
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Tidskriftsartikel (refereegranskat)abstract
- 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 multiconfigurational 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 [C. Froese Fischer et al., Comput. Phys. Commun. 176, 559 (2007)]. 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 3s3p(6)np 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 Guenot et al. [Phys. Rev. A 85, 053424 (2012)]. The effect of the presence of resonances in the one-photon spectrum on photoionization delay measurements is studied. DOI: 10.1103/PhysRevA.87.023420
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| 6. |
- Dahlström, J. Marcus, et al.
(författare)
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Diagrammatic approach to attosecond delays in photoionization
- 2012
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 86:6, s. 061402-
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Tidskriftsartikel (refereegranskat)abstract
- We study laser-assisted photoionization by attosecond pulses using a time-independent formalism based on diagrammatic many-body perturbation theory. Our aim is to provide an ab initio route to the delays for this above-threshold ionization process, which is essential for a quantitative understanding of attosecond metrology. We present correction curves for characterization schemes of attosecond pulses, such as streaking, that account for the delayed atomic response in ionization from neon and argon. We also verify that photoelectron delays from many-electron atoms can be measured using similar schemes if, instead, the so-called continuum-continuum delay is subtracted. Our method is general and it can be extended also to more complex systems and additional correlation effects can be introduced systematically. DOI: 10.1103/PhysRevA.86.061402
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| 7. |
- Dahlström, J. Marcus, et al.
(författare)
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Introduction to attosecond delays in photoionization
- 2012
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 45:18, s. 183001-
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Tidskriftsartikel (refereegranskat)abstract
- This tutorial presents an introduction to the interaction of light and matter on the attosecond timescale. Our aim is to detail the theoretical description of ultra-short time delays and to relate these to the phase of extreme ultraviolet (XUV) light pulses and to the asymptotic phaseshifts of photoelectron wave packets. Special emphasis is laid on time-delay experiments, where attosecond XUV pulses are used to photoionize target atoms at well-defined times, followed by a probing process in real time by a phase-locked, infrared laser field. In this way, the laser field serves as a 'clock' to monitor the ionization event, but the observable delays do not correspond directly to the delay associated with single-photon ionization. Instead, a significant part of the observed delay originates from a measurement induced process, which obscures the single-photon ionization dynamics. This artefact is traced back to a phaseshift of the above-threshold ionization transition matrix element, which we call the continuum-continuum phase. It arises due to the laser-stimulated transitions between Coulomb continuum states. As we shall show here, these measurement-induced effects can be separated from the single-photon ionization process, using analytical expressions of universal character, so that eventually the attosecond time delays in photoionization can be accessed.
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| 8. |
- Dahlström, J. Marcus, et al.
(författare)
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Photoionization Time Delays
- 2016
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Ingår i: Ultrafast Dynamics Driven by Intense Light Pulses. - Cham : Springer. - 9783319201726 - 9783319201733 ; , s. 177-202
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Bokkapitel (refereegranskat)abstract
- The material presented in this chapter is based on important advances realized in attophysics which make feasible to follow the motion of electrons in atoms and molecules with attosecond-level time resolution. In this context, time-delays have been recently determined in the process of photoionization by extreme-ultra- violet (XUV) pulses and the question of the significance of these measured delays arises. As we shall outline here, numerical experiments show that they are intimately related to the structure of the ionized species' continuous spectrum. Another point addressed here is that, in experiments, the measurements have the common characteristic to be performed in the presence of an auxiliary infra-red (IR) field, used to clock the timing of the process. This implies to adapt the theory treatment to handle such two-color photoionization processes. We review a systematic analysis of these features that are characteristic of this class of electronic transitions, when viewed in the time domain.
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| 9. |
- Dahlström, J. Marcus, et al.
(författare)
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Study of attosecond delays using perturbation diagrams and exterior complex scaling
- 2014
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 47:12, s. 124012-
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Tidskriftsartikel (refereegranskat)abstract
- We describe in detail how attosecond delays in laser-assisted photoionization can be computed using perturbation theory based on two-photon matrix elements. Special emphasis is laid on above-threshold ionization, where the electron interacts with an infrared field after photoionization by an extreme ultraviolet field. Correlation effects are introduced using diagrammatic many-body theory to the level of the random-phase approximation with exchange. Our aim is to provide an ab initio route to correlated multi-photon processes that are required for an accurate description of experiments on the attosecond time scale. Here, our results are focused on photoionization of the M-shell of argon atoms, where experiments have been carried out using the so-called reconstruction of attosecond beating by the two-photon interference transitions technique. An influence of autoionizing resonances in attosecond delay measurements is observed. Further, it is shown that the delay depends on both detection angle of the photoelectron and energy of the probe photon.
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| 10. |
- Dahlström, J. Marcus, 1982-, et al.
(författare)
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Theory of attosecond delays in laser-assisted photoionization
- 2013
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Ingår i: Chemical Physics. - : Elsevier BV. - 0301-0104 .- 1873-4421. ; 414, s. 53-64
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Tidskriftsartikel (refereegranskat)abstract
- We study the temporal aspects of laser-assisted extreme ultraviolet (XUV) photoionization using attosecond pulses of harmonic radiation. The aim of this paper is to establish the general form of the phase of the relevant transition amplitudes and to make the connection with the time-delays that have been recently measured in experiments. We find that the overall phase contains two distinct types of contributions: one is expressed in terms of the phase-shifts of the photoelectron continuum wavefunction while the other is linked to continuum–continuum transitions induced by the infrared (IR) laser probe. Our formalism applies to both kinds of measurements reported so far, namely the ones using attosecond pulse trains of XUV harmonics and the others based on the use of isolated attosecond pulses (streaking). The connection between the phases and the time-delays is established with the help of finite difference approximations to the energy derivatives of the phases. The observed time-delay is a sum of two components: a one-photon Wigner-like delay and an universal delay that originates from the probing process itself.
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| 11. |
- Guenot, Diego, et al.
(författare)
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Measurements of relative photoemission time delays in noble gas atoms
- 2014
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 47:24, s. 245602-
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Tidskriftsartikel (refereegranskat)abstract
- We determine relative photoemission time delays between valence electrons in different noble gas atoms (Ar, Ne and He) in an energy range between 31 and 37 eV. The atoms are ionized by an attosecond pulse train synchronized with an infrared laser field and the delays are measured using an interferometric technique. We compare our results with calculations using the random phase approximation with exchange and multi-configurational Hartree-Fock. We also investigate the influence of the different ionization angular channels.
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| 12. |
- Guenot, Diego, et al.
(författare)
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Photoemission time delay measurements and calculations close to the 3s ionization cross section minimum in ar
- 2012
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Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 85:5, s. 053424-
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Tidskriftsartikel (refereegranskat)abstract
- We present experimental measurements and theoretical calculations of photoionization time delays from the 3s and 3p shells in Ar in the photon energy range of 32-42 eV. The experimental measurements are performed by interferometry using attosecond pulse trains and the infrared laser used for their generation. The theoretical approach includes intershell correlation effects between the 3s and 3p shells within the framework of the random-phase approximation with exchange. The connection between single-photon ionization and the two-color two-photon ionization process used in the measurement is established using the recently developed asymptotic approximation for the complex transition amplitudes of laser-assisted photoionization. We compare and discuss the theoretical and experimental results, especially in the region where strong intershell correlations in the 3s -> kp channel lead to an induced Cooper minimum in the 3s ionization cross section.
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| 13. |
- Heuser, Sebastian, et al.
(författare)
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Angular dependence of photoemission time delay in helium
- 2016
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Ingår i: Physical Review A. - 2469-9926. ; 94:6
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Tidskriftsartikel (refereegranskat)abstract
- 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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| 14. |
- Jiang, Wenyu, et al.
(författare)
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Resolving Quantum Interference Black Box through Attosecond Photoionization Spectroscopy
- 2023
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Ingår i: Physical Review Letters. - 0031-9007. ; 131:20
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Tidskriftsartikel (refereegranskat)abstract
- Multiphoton light-matter interactions invoke a so-called "black box"in which the experimental observations contain the quantum interference between multiple pathways. Here, we employ polarization-controlled attosecond photoelectron metrology with a partial wave manipulator to deduce the pathway interference within this quantum 'black box"for the two-photon ionization of neon atoms. The angle-dependent and attosecond time-resolved photoelectron spectra are measured across a broad energy range. Two-photon phase shifts for each partial wave are reconstructed through the comprehensive analysis of these photoelectron spectra. We resolve the quantum interference between the degenerate p→d→p and p→s→p two-photon ionization pathways, in agreement with our theoretical simulations. Our approach thus provides an attosecond time-resolved microscope to look inside the "black box"of pathway interference in ultrafast dynamics of atoms, molecules, and condensed matter.
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| 15. |
- Klünder, Kathrin, et al.
(författare)
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Probing Single-Photon Ionization on the Attosecond Time Scale
- 2011
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Ingår i: Physical Review Letters. - 1079-7114. ; 106:14
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Tidskriftsartikel (refereegranskat)abstract
- We study photoionization of argon atoms excited by attosecond pulses using an interferometric measurement technique. We measure the difference in time delays between electrons emitted from the 3s(2) and from the 3p(6) shell, at different excitation energies ranging from 32 to 42 eV. The determination of photoemission time delays requires taking into account the measurement process, involving the interaction with a probing infrared field. This contribution can be estimated using a universal formula and is found to account for a substantial fraction of the measured delay.
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| 16. |
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| 17. |
- Kotur, Marija, et al.
(författare)
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Spectral phase measurement of a Fano resonance using tunable attosecond pulses
- 2016
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 7
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Tidskriftsartikel (refereegranskat)abstract
- Electron dynamics induced by resonant absorption of light is of fundamental importance in nature and has been the subject of countless studies in many scientific areas. Above the ionization threshold of atomic or molecular systems, the presence of discrete states leads to autoionization, which is an interference between two quantum paths: direct ionization and excitation of the discrete state coupled to the continuum. Traditionally studied with synchrotron radiation, the probability for autoionization exhibits a universal Fano intensity profile as a function of excitation energy. However, without additional phase information, the full temporal dynamics cannot be recovered. Here we use tunable attosecond pulses combined with weak infrared radiation in an interferometric setup to measure not only the intensity but also the phase variation of the photoionization amplitude across an autoionization resonance in argon. The phase variation can be used as a fingerprint of the interactions between the discrete state and the ionization continua, indicating a new route towards monitoring electron correlations in time.
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| 18. |
- Mansten, Erik, et al.
(författare)
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Spectral signature of short attosecond pulse trains.
- 2009
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Ingår i: Physical Review Letters. - 1079-7114. ; 102:8
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Tidskriftsartikel (refereegranskat)abstract
- We report experimental measurements of high-order harmonic spectra generated in Ar using a carrier-envelope-offset (CEO) stabilized 12 fs, 800 nm laser field and a fraction (less than 10%) of its second harmonic. Additional spectral peaks are observed between the harmonic peaks, which are due to interferences between multiple pulses in the train. The position of these peaks varies with the CEO and their number is directly related to the number of pulses in the train. An analytical model, as well as numerical simulations, support our interpretation.
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| 19. |
- Nandi, Saikat, et al.
(författare)
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Generation of entanglement using a short-wavelength seeded free-electron laser
- 2024
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Ingår i: SCIENCE ADVANCES. - 2375-2548. ; 10:16
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Tidskriftsartikel (refereegranskat)abstract
- Quantum entanglement between the degrees of freedom encountered in the classical world is challenging to observe due to the surrounding environment. To elucidate this issue, we investigate the entanglement generated over ultrafast timescales in a bipartite quantum system comprising two massive particles: a free-moving photoelectron, which expands to a mesoscopic length scale, and a light-dressed atomic ion, which represents a hybrid state of light and matter. Although the photoelectron spectra are measured classically, the entanglement allows us to reveal information about the dressed-state dynamics of the ion and the femtosecond extreme ultraviolet pulses delivered by a seeded free-electron laser. The observed generation of entanglement is interpreted using the time-dependent von Neumann entropy. Our results unveil the potential for using short-wavelength coherent light pulses from free-electron lasers to generate entangled photoelectron and ion systems for studying spooky action at a distance.
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| 20. |
- Nandi, Saikat, et al.
(författare)
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Observation of Rabi dynamics with a short-wavelength free-electron laser
- 2022
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Ingår i: Nature. - : Springer Science and Business Media LLC. - 0028-0836 .- 1476-4687. ; 608:7923
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Tidskriftsartikel (refereegranskat)abstract
- Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field(1). They are ubiquitous in physics with applications in different areas such as photonics(2), nano-electronics(3), electron microscopy(4) and quantum information(5). While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light-matter interactions within the rotating-wave approximation(6). Although intense nanometre-wavelength light sources have been available for more than a decade(7-9), Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser(10) can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler-Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom-field interactions(11). Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond(12) and few-femtosecond(13) extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.
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| 21. |
- Nandi, Saikat, et al.
(författare)
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Unraveling Rabi dynamics with a seeded FEL at XUV wavelength
- 2023
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Ingår i: 2023 Conference on Lasers and Electro-Optics Europe and European Quantum Electronics Conference, CLEO/Europe-EQEC 2023. - 9798350345995
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Konferensbidrag (refereegranskat)abstract
- Rabi oscillations, a prominent feature of coherent light-matter interaction arise when a two-level system interacts periodically with an external electromagnetic field [1]. Despite being a cornerstone in quantum physics, they are usually studied in the long-wavelength region, ranging from mid-infrared to visible. Here, we demonstrate that intense femtosecond extreme-ultraviolet (XUV) pulses from FERMI seeded free-electron laser [2] can drive Rabi oscillations between the two levels: 1s2 and 1s4p in helium.
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| 22. |
- Palatchi, Caryn, et al.
(författare)
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Atomic delay in helium, neon, argon and krypton
- 2014
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 47:24, s. 245003-
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Tidskriftsartikel (refereegranskat)abstract
- Photoionization by an eXtreme UltraViolet (XUV) attosecond pulse train (APT) in the presence of an infrared pulse (RABBITT method) conveys information about the atomic photoionization delay. By taking the difference of the spectral delays between pairs of rare gases (Ar,He), (Kr,He) and (Ne,He) it is possible to eliminate in each case the larger group delay ('attochirp') associated with the APT itself and obtain the Ar, Kr and Ne Wigner delays referenced to model calculations of the He delay. In this work we measure how the delays vary as a function of XUV photon energy but we cannot determine the absolute delay difference between atoms due to lack of precise knowledge of the initial conditions. The extracted delays are compared with several theoretical predictions and the results are consistent within 30 as over the energy range from 10 to 50 eV. An 'effective' Wigner delay over all emission angles is found to be more consistent with our angle-integrated measurement near the Cooper minimum in Ar. We observe a few irregular features in the delay that may be signatures of resonances.
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| 23. |
- Swoboda, Marko, et al.
(författare)
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Intensity dependence of laser-assisted attosecond photoionization spectra
- 2009
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Ingår i: Laser Physics. - 1054-660X. ; 19:8, s. 1591-1599
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Tidskriftsartikel (refereegranskat)abstract
- We study experimentally the influence of the intensity of the infrared (IR) probe field on attosecond pulse train (APT) phase measurements performed with the RABITT method (Reconstruction of Attosecond Beating by Interference in Two-Photon Transitions). We find that if a strong IR field is applied, the attosecond pulses will appear to have lower-than-actual chirp rates. We also observe the onset of the streaking regime in the breakdown of the weak-field RABITT conditions. We perform a Fourier-analysis of harmonic and sideband continuum states and show that the mutual phase relation of the harmonics can be extracted from higher Fourier components.
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| 24. |
- Swoboda, Marko, et al.
(författare)
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Phase Measurement of Resonant Two-Photon Ionization in Helium
- 2010
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Ingår i: Physical Review Letters. - 1079-7114. ; 104:10
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Tidskriftsartikel (refereegranskat)abstract
- We study resonant two-color two-photon ionization of helium via the 1s3p P-1(1) state. The first color is the 15th harmonic of a tunable Ti:sapphire laser, while the second color is the fundamental laser radiation. Our method uses phase-locked high-order harmonics to determine the phase of the two-photon process by interferometry. The measurement of the two-photon ionization phase variation as a function of detuning from the resonance and intensity of the dressing field allows us to determine the intensity dependence of the transition energy.
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