Space–time control of free induction decay in the extreme ultraviolet

Bengtsson, Samuel; Larsen, Esben W.; Kroon, David; Camp, Seth; Miranda, Miguel; Arnold, Cord L.; L’Huillier, Anne; Schafer, Kenneth J.; Gaarde, Mette B.; Rippe, Lars; Mauritsson, Johan

doi:10.1038/nphoton.2017.30

Cited by 73 publications

(57 citation statements)

References 45 publications

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“…Spatially offsetting a smaller pump beam and a larger probe beam imprints an approximately linear phase gradient across the pump beam so that all the np emission is redirected in the same direction, as observed in Refs. [8,9] [upward in Fig. 2(a)].…”

Section: Principlementioning

confidence: 99%

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Probing Stark-induced nonlinear phase variation with opto-optical modulation

Simpson¹,

Labeye

Camp

et al. 2019

Phys. Rev. A

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We extend the recently developed technique of opto-optical modulation (OOM) to probe stateresolved ac-Stark-induced phase variations of a coherently excited ensemble of helium atoms. In a joint experimental and theoretical study, we find that the spatial redirection of the resonant emission from the OOM process is different for the low-lying 1s2p state as compared with the higher-lying Rydberg states, and that this redirection can be controlled through the spatial characteristics of the infrared (IR) probe beam. In particular, we observe that the intensity dependence of the IR-induced Stark phase on the 1s2p emission is nonlinear, and that the phase accumulation changes sign for moderate intensities. Our results suggest that OOM, combined with precise experimental shaping of the probe beam, could allow future measurements of Stark-induced phase shifts of excited states.

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Section: Principlementioning

confidence: 99%

“…Previously OOM has been used to redirect ultrafast XUV light pulses in an argon gas, from both Rydberg and autoionizing states [8,9]. Further details of the technique using also helium and neon gases can be found in Ref.…”

Section: Introductionmentioning

confidence: 99%

Probing Stark-induced nonlinear phase variation with opto-optical modulation

Simpson¹,

Labeye

Camp

et al. 2019

Phys. Rev. A

Self Cite

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“…This laser-induced phase was shown to enable full control over the absorption lineshapes, from Lorentz to Fano profiles [13]. This effect was also used to spatially deflect the XFID radiation by creating a Stark-shift gradient in the medium [14]. The combination of these different physical effects and observables provides a very rich framework for ultrafast spectroscopy and strong-field physics, enabling for instance the complete reconstruction of a two-electron wavepackets [15].…”

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confidence: 99%

Phase-resolved two-dimensional spectroscopy of electronic wave packets by laser-induced XUV free induction decay

et al. 2017

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We present a novel time-and phase-resolved, background-free scheme to study the extreme ultraviolet dipole emission of a bound electronic wavepacket, 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.Transient Absorption Spectroscopy (TAS) in the extreme ultraviolet (XUV) range is a powerful technique for ultrafast dynamical studies, from the gas phase [1][2][3] to the solid state [4,5]. The recent progress of attosecond science has made the extension of TAS to the attosecond regime (ATAS) a reality. In the past few years, different configurations of ATAS experiments have emerged. In the first and most intuitive scheme, the XUV attosecond pulses probe a sample that has been pre-excited by an infrared (IR) pump laser pulse. This scheme was for instance used to follow the ultrafast coherent hole dynamics initiated in strong-field ionized krypton [1]. In the second arrangement, the XUV and IR pulses are temporally overlapped. The XUV absorption thus probes the IR-dressed atomic or molecular states, allowing the observation of light-induced states [6,7] as well as sub-cycle AC-Stark-shifts [8]. Finally, in what turned out to be the most widely used scheme, the XUV pulse comes first and serves as a pump, exciting a broadband superposition of quantum states through single-photon absorption. The wavepacket relaxes by coherently emitting XUV radiation (called XUV Free Induction Decay, XFID) that interferes with the incident light. A delayed IR laser field is used to follow or control the relaxation dynamics, such that these experiments can be seen as Transient Reshaping of the Absorption spectrum of the XUV light (TRAX) [9,10].In TRAX experiments, the delayed IR laser pulse has three main effects on the XFID emission ( Fig. 1) : (i) Damping of the emission by ionization of the excited states. This effect induces a lowering and a spectral broadening of the absorption features [2]. (ii) Field coupling of different electronic states, leading to population transfers. The resulting amplitude reshaping of the electronic wavepacket can be detected through temporal beatings in the absorption signal, as demonstrated in atoms [9,10] and molecules [11,12]. (iii) Phase shift induced by the Stark-shift of the excited states. This laser-induced phase was shown to enable full control over the absorption lineshapes, from Lorentz ...

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“…One of the core assumptions of the SFA is to neglect the influence of bound excited states in the highharmonic generation. However, as experiments get more sophisticated, coherent XUV emission processes involving these states are being discovered and investigated: XUV free-induction decay, either excited by singlephoton [5,6] or multiphoton absorption [7], high-order harmonic generation (HHG) from excited Rydberg states [8] or from frustrated tunnel ionization [9]. The XUV emission constitutes a spectroscopic signature of the strong-field dynamics involving the bound excited states, and could thus be used to resolve their dynamics.…”

Section: Introductionmentioning

confidence: 99%

“…A scheme of the simultaneous generation of high-order harmonics and HRL is shown in figure 1(a). The creation of a coherence between the ground state and an excited state can also lead to emission features from the Free-Induction Decay process in the XUV range (xFID) [5,7].…”

Section: Introductionmentioning

confidence: 99%

Hyper-Raman lines emission concomitant with high-order harmonic generation

et al. 2019

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Hyper-Raman lines (HRL) resulting from strong-field light-matter interaction have been predicted theoretically in the 1990s but never identified in high-order harmonic generation experiments. Here, we use a combination of 800 and 400 nm laser pulses to control independently the two processes required for the hyper-Raman emission: creation of a coherence between two electronic states and laser-dressing of these states. As a result we observe simultaneously high-order harmonics, XUV free induction decay and HRL. We investigate experimentally and numerically the properties of this novel emission source. It can be of high interest, amongst others, for high-resolution spatio-temporal spectroscopy of excited electronic states in the same fashion high-order harmonics generation provides it for ground state.

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Space–time control of free induction decay in the extreme ultraviolet

Cited by 73 publications

References 45 publications

Probing Stark-induced nonlinear phase variation with opto-optical modulation

Probing Stark-induced nonlinear phase variation with opto-optical modulation

Phase-resolved two-dimensional spectroscopy of electronic wave packets by laser-induced XUV free induction decay

Hyper-Raman lines emission concomitant with high-order harmonic generation

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