Near-resonant four-wave mixing of attosecond extreme-ultraviolet pulses with near-infrared pulses in neon: Detection of electronic coherences

Cao, Wei; Warrick, Erika R.; Fidler, Ashley; Leone, Stephen R.; Neumark, Daniel M.

doi:10.1103/physreva.94.021802

Cited by 49 publications

(56 citation statements)

References 35 publications

(39 reference statements)

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“…More generally, the investigation of the fast beatings shows the ability of T-REX to provide high-quality data for 2D spectroscopy. This scheme is conceptually similar to the XUV-IR four-wave mixing experiments recently demonstrated [21], and could be extended by using more sophisticated spatial and temporal combinations of excitation and probe pulses [22].…”

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confidence: 96%

“…Pressure dependences have also been observed in absorption spectra and TRAX experiments. They have been interpreted as resulting from the reshaping of the propagating XUV exciting pulse by the strongly dispersive absorbing medium [21]. While these effects certainly have an influence in TRAX, they cannot be at play in T-REX which is based on multiphoton excitation by VIS pulses.…”

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confidence: 99%

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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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confidence: 96%

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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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“…In this paper, the dynamics of an XUV-excited vibronic wavepacket in a prototypical molecular system, H 2 , is explored. The recently developed method of XUV/near-infrared (NIR) four wave mixing spectroscopy [13][14]is applied to characterize the many pathways from the interaction of the NIR field with the XUV-excited state, probing such effects as laser-driven electronic-nuclear correlation and quantum coherence of the molecular wavepacket.…”

Section: Introductionmentioning

confidence: 99%

“…Recently, it has been shown that by crossing an XUV attosecond pulse with a NIR laser pulse at a small angle, nonlinear XUV-NIR four wave mixing (FWM) from anatomic gas medium is observed at different emitting angles determined by the phase matching conditions [13]. Under such a non-collinear geometry, ultrafast XUV spectroscopy gains an additional dimension that is angle-resolved.…”

Section: Introductionmentioning

confidence: 99%

Excited-state vibronic wave-packet dynamics in H2 probed by XUV transient four-wave mixing

et al. 2018

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The complex behavior of a molecular wavepacket initiated by an extreme ultraviolet (XUV)pulse is investigated with noncollinear wave mixing spectroscopy. A broadband XUV pulse spanning 12eV to 16eV launches a wavepacket in H 2 comprising a coherent superposition of multiple electronic and vibrational levels.The molecular wavepacket evolves freely until a delayed few-cycle optical laser pulse arrives to induce nonlinear signals in the XUV via four wave mixing (FWM). The angularly resolved FWM signals encode rich energy exchange processes between the optical laser field and the XUV excited molecule. The non-collinear geometry enables spatial separation of ladder and vee/lambda-type transitions induced by the optical field. Ladder transitions, in which the energy exchange with the optical field is around 3 eV, appear off-axis from the incident XUV beam. Each vibrationally revolved FWM line probes a different part of the wavepacket in energy, serving as a promising tool for energetic tomography of molecular wavepackets. Vee/lambda-type transitions, in which the energy exchange is well under 1 eV, result in on-axis nonlinear signals. The first order versus third order interference of the on-axis signal serves as a mapping tool of the energy flow pathways. Intra and inter electronic potential energy curve (PEC) transitions are decisively identified. The current study opens possibilities for accessing complete dynamic information in XUV excited complex systems.

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“…In the past decades, femtosecond laser pulses have become effective tools in various fields including high-order harmonic generation (HHG) [1][2][3][4][5][6], strong-field ionization [6][7][8][9][10][11][12][13][14][15][16][17], and time-resolved spectroscopy [18][19][20][21][22][23][24] due to their ultrashort pulse duration and high peak intensity. Benefiting from the Kerr lens mode-locking (KLM) [25,26] and chirped pulse amplification (CPA) [27][28][29], the Ti:sapphire lasers have developed rapidly towards shorter pulse durations and higher pulse energies.…”

Section: Introductionmentioning

confidence: 99%

Ultrafast Mid-IR Laser Pulses Generation via Chirp Manipulated Optical Parametric Amplification

et al. 2018

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Abstract:Over the past decades, optical parametric amplification (OPA) has become one of the most promising sources of ultrafast Mid-IR laser, owing to its outstanding properties including ultrabroad bandwidth, superior tunability, good beam quality, and scalable energy. In this paper, we review the recent progress in ultrashort laser pulse generation via chirp manipulated OPA, which improves the energy scalability and gain bandwidth by strategically chirping both pump and seed pulses. The gain mechanism is theoretically analyzed and the OPA processes are numerically simulated. In addition, the concept is verified experimentally. Femtosecond pulses with hundreds of mJ are generated in a high energy dual-chirped-OPA (DC-OPA), and ultrabroadband µJ-level spectra supporting sub-2-cycle pulse durations are achieved in BBP-OPA. Furthermore, the obtained pulses show excellent tunability through the NIR to Mid-IR regions, which makes them a suitable seeding source for further amplification as well as powerful tools in various applications such as strong field physics, attosecond science, and ultrafast spectroscopy.

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Near-resonant four-wave mixing of attosecond extreme-ultraviolet pulses with near-infrared pulses in neon: Detection of electronic coherences

Cited by 49 publications

References 35 publications

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

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

Excited-state vibronic wave-packet dynamics in H2 probed by XUV transient four-wave mixing

Ultrafast Mid-IR Laser Pulses Generation via Chirp Manipulated Optical Parametric Amplification

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