Autoionization Dynamics of (2P1/2)ns/d States in Krypton Probed by Noncollinear Wave Mixing with Attosecond Extreme Ultraviolet and Few-Cycle Near Infrared Pulses

The autoionization dynamics of the (2P1/2)ns/d Rydberg states in krypton are investigated using wave-mixing signals generated with subfemtosecond XUV pulses and noncollinear, few-cycle NIR pulses. Despite quantum beat oscillations from the XUV-induced coherence, these wave-mixing spectra allow for the simultaneous evaluation of autoionization lifetimes from a series of Rydberg states. Experimentally measured lifetimes for the wave-mixing signals emitting from the (2P1/2)6d/8s, 7d/9s, and 8d/10s resonances compare favorably with lifetimes for the (2P1/2)6d, 7d, and 8d Rydberg states determined from spectral linewidths. Analysis of the quantum beats reveals that the enhancement of wave-mixing pathways leads to reporter state-dependent decays in the wave-mixing signals. The results demonstrate the promise of wave-mixing spectroscopies with subfemtosecond XUV pulses to provide valuable insights into processes governed by electronic dynamics.

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Multidimensional spectroscopy with attosecond extreme ultraviolet and shaped near-infrared pulses

Science Advances ◽

10.1126/sciadv.aau3783 ◽

2018 ◽

Vol 4 (9) ◽

pp. eaau3783 ◽

Cited By ~ 16

Author(s):

Hugo J. B. Marroux ◽

Ashley P. Fidler ◽

Daniel M. Neumark ◽

Stephen R. Leone

Keyword(s):

Excited States ◽

Near Infrared ◽

Extreme Ultraviolet ◽

Four Wave Mixing ◽

High Dimensionality ◽

Wave Mixing ◽

Multidimensional Spectroscopy ◽

Electronic Dynamics ◽

Single State ◽

Signal Field

Dynamics following excitation with attosecond extreme ultraviolet (XUV) pulses arise from enormous numbers of accessible excited states, complicating the retrieval of state-specific time evolutions. We develop attosecond XUV multidimensional spectroscopy here to separate interfering pathways on a near-infrared (NIR) energy axis, retrieving single state dynamics in argon atoms in a two-dimensional (2D) XUV-NIR spectrum. In this experiment, we measure four-wave mixing signal arising from the interaction of XUV attosecond pulses centered around 15 eV with two few-cycle NIR pulses. The 2D spectrum is created by measuring the emitted XUV signal field spectrum while applying narrowband amplitude and phase modulations to one of the NIR pulses. Application of such a technique to systems of high dimensionality will provide for the observation of state-resolved pure electronic dynamics, in direct analogy to phenomena unraveled by multidimensional spectroscopies at optical frequencies.

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Zeeman quantum beats of helium Rydberg states excited by synchrotron radiation

Journal of Synchrotron Radiation ◽

10.1107/s1600577520002829 ◽

2020 ◽

Vol 27 (3) ◽

pp. 675-680 ◽

Cited By ~ 2

Author(s):

Yasumasa Hikosaka ◽

Hiroshi Iwayama ◽

Tatsuo Kaneyasu

Keyword(s):

Synchrotron Radiation ◽

Ultraviolet Light ◽

Extreme Ultraviolet ◽

Rydberg States ◽

Fluorescence Decay ◽

Quantum Beat ◽

Quantum Beats ◽

Theoretical Formulation ◽

Polarization Characteristics ◽

Extreme Ultraviolet Light

Quantum beats in fluorescence decay from Zeeman-split magnetic sublevels have been measured for helium Rydberg states excited by synchrotron radiation. The Zeeman quantum beats observed in this prototypical case were fitted with an equation from a theoretical formulation. It is proposed that Zeeman quantum beat measurement can be a useful way to simply evaluate the polarization characteristics of extreme ultraviolet light.

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

Physical Review A ◽

10.1103/physreva.94.021802 ◽

2016 ◽

Vol 94 (2) ◽

Cited By ~ 21

Author(s):

Wei Cao ◽

Erika R. Warrick ◽

Ashley Fidler ◽

Stephen R. Leone ◽

Daniel M. Neumark

Keyword(s):

Near Infrared ◽

Extreme Ultraviolet ◽

Four Wave Mixing ◽

Wave Mixing

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Autoionization dynamics of (2P1/2)ns/d states in krypton probed by noncollinear wave mixing with attosecond extreme ultraviolet and few-cycle near infrared pulses

The Journal of Chemical Physics ◽

10.1063/1.5113912 ◽

2019 ◽

Vol 151 (11) ◽

pp. 114305 ◽

Cited By ~ 4

Author(s):

Ashley P. Fidler ◽

Hugo J. B. Marroux ◽

Erika R. Warrick ◽

Etienne Bloch ◽

Wei Cao ◽

...

Keyword(s):

Near Infrared ◽

Extreme Ultraviolet ◽

Wave Mixing

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Study of Multiple Quantum Beats in Atomic Wavepackets

Applied Mechanics and Materials ◽

10.4028/www.scientific.net/amm.325-326.119 ◽

2013 ◽

Vol 325-326 ◽

pp. 119-122

Author(s):

Chang Jun Zhu ◽

Bing Xue ◽

Xue Jun Zhai ◽

Jun Fang He

Keyword(s):

Density Matrix ◽

Four Wave Mixing ◽

Quantum Beat ◽

System Response ◽

Quantum Beats ◽

Multiple Quantum ◽

Wave Mixing ◽

Third Order ◽

Mixing Processes ◽

The Third

A theoretical model consisting of 5 energy levels in coupled four-wave mixing processes was proposed to analyze the coherent characteristics of atomic wavepackets using perturbative theory. The equations of motions of the density matrix were derived and the third-order density matrix elements were presented. Under the condition that the duration of laser pulses is sufficiently short, the system response was treated as impulse response. Moreover, in the lowest order perturbation theory, the third-order nonlinear polarization was obtained using rotating-wave approximation. The results show that multiple quantum beats are embedded in the coupled four-wave mixing signals, and coherent dynamics of wavepackets can be retrieved from the quantum beat dynamics.

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Coherence tomography with broad bandwidth extreme ultraviolet and soft X-ray radiation

Applied Physics B ◽

10.1007/s00340-021-07586-w ◽

2021 ◽

Vol 127 (4) ◽

Author(s):

S. Skruszewicz ◽

S. Fuchs ◽

J. J. Abel ◽

J. Nathanael ◽

J. Reinhard ◽

...

Keyword(s):

Optical Coherence Tomography ◽

Near Infrared ◽

Extreme Ultraviolet ◽

Infrared Light ◽

Imaging Method ◽

Optical Coherence ◽

Axial Resolution ◽

Cross Sectional ◽

X Ray ◽

Broad Bandwidth

AbstractWe present an overview of recent results on optical coherence tomography with the use of extreme ultraviolet and soft X-ray radiation (XCT). XCT is a cross-sectional imaging method that has emerged as a derivative of optical coherence tomography (OCT). In contrast to OCT, which typically uses near-infrared light, XCT utilizes broad bandwidth extreme ultraviolet (XUV) and soft X-ray (SXR) radiation (Fuchs et al in Sci Rep 6:20658, 2016). As in OCT, XCT’s axial resolution only scales with the coherence length of the light source. Thus, an axial resolution down to the nanometer range can be achieved. This is an improvement of up to three orders of magnitude in comparison to OCT. XCT measures the reflected spectrum in a common-path interferometric setup to retrieve the axial structure of nanometer-sized samples. The technique has been demonstrated with broad bandwidth XUV/SXR radiation from synchrotron facilities and recently with compact laboratory-based laser-driven sources. Axial resolutions down to 2.2 nm have been achieved experimentally. XCT has potential applications in three-dimensional imaging of silicon-based semiconductors, lithography masks, and layered structures like XUV mirrors and solar cells.

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State-selective quantum beat spectroscopy via coherent control of Liouville-pathway interference in two-colour resonant four-wave mixing

Journal of Physics B Atomic Molecular and Optical Physics ◽

10.1088/0953-4075/32/18/301 ◽

1999 ◽

Vol 32 (18) ◽

pp. 4389-4404 ◽

Cited By ~ 7

Author(s):

F Di Teodoro ◽

E F McCormack

Keyword(s):

Coherent Control ◽

Four Wave Mixing ◽

Quantum Beat ◽

Wave Mixing

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A Versatile Setup for Time-Resolved Functional Near Infrared Spectroscopy Based on Fast-Gated Single-Photon Avalanche Diode and on Four-Wave Mixing Laser

Applied Sciences ◽

10.3390/app9112366 ◽

2019 ◽

Vol 9 (11) ◽

pp. 2366 ◽

Cited By ~ 2

Author(s):

Laura Di Sieno ◽

Alberto Dalla Mora ◽

Alessandro Torricelli ◽

Lorenzo Spinelli ◽

Rebecca Re ◽

...

Keyword(s):

Infrared Spectroscopy ◽

Near Infrared Spectroscopy ◽

Near Infrared ◽

Single Photon ◽

Wave Mixing ◽

Functional Near Infrared Spectroscopy ◽

Time Resolved ◽

Diffusive Medium ◽

Spectroscopy System

In this paper, a time-domain fast gated near-infrared spectroscopy system is presented. The system is composed of a fiber-based laser providing two pulsed sources and two fast gated detectors. The system is characterized on phantoms and was tested in vivo, showing how the gating approach can improve the contrast and contrast-to-noise-ratio for detection of absorption perturbation inside a diffusive medium, regardless of source-detector separation.

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