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

Marroux, Hugo J. B.; Fidler, Ashley; Neumark, Daniel M.; Leone, Stephen R.

doi:10.1126/sciadv.aau3783

Cited by 43 publications

(39 citation statements)

References 23 publications

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“…Single state dynamics can be retrieved by again using a technique widely used in the visible and Mid-IR. Marroux et al developed a multidimensional spectroscopy in the XUV that provides frequency resolution on the NIR interaction energy while preserving the experiment time resolution [63]. Fig.…”

Section: I-3 N Wave Mixing Spectroscopymentioning

confidence: 99%

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Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids

Géneaux

Marroux

Guggenmos

et al. 2019

Phil. Trans. R. Soc. A.

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Attosecond science opened the door to observing nuclear and electronic dynamics in real time and has begun to expand beyond its traditional grounds. Among several spectroscopic techniques, X-ray transient absorption spectroscopy has become key in understanding matter on ultrafast time scales. In this review, we illustrate the capabilities of this unique tool through a number of iconic experiments. We outline how coherent broadband X-ray radiation, emitted in high-harmonic generation, can be used to follow dynamics in increasingly complex systems. Experiments performed in both molecules and solids are discussed at length, on time scales ranging from attoseconds to picoseconds, and in perturbative or strong-field excitation regimes. This article is part of the theme issue ‘Measurement of ultrafast electronic and structural dynamics with X-rays’.

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Section: I-3 N Wave Mixing Spectroscopymentioning

confidence: 99%

“…The experimental time traces of the 4WM signal, when probing either the inner or outer well, are shown below. (b) Two-dimensional spectroscopy at XUV energies [63]. The camera image and time evolution of the 1D measurement are shown along with the state labeling.…”

Section: Perspectives For Attosecond Spectroscopymentioning

confidence: 99%

Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids

Géneaux

Marroux

Guggenmos

et al. 2019

Phil. Trans. R. Soc. A.

Self Cite

201

147

View full text Add to dashboard Cite

show abstract

“…Capitalizing on the phasematching conditions inherent in wave-mixing processes, recent experiments employed a noncollinear beam geometry between an XUV attosecond pulse train and either one [28,29] or two [30][31][32] moderately intense NIR pulses to measure transient spectra of spatially isolated XUV wave-mixing signals. These time-dependent wave-mixing signals were utilized to characterize a dark state in N2 [30], to measure ultrafast lifetimes of autoionizing states in krypton [32], and to construct the first multidimensional spectrum in the XUV by implementing NIR pulse shaping techniques [33]. While highly versatile, these noncollinear wave-mixing measurements are typically best described as homodyne techniques [32], and therefore do not benefit from the signal enhancement and phase-sensitivity characteristic of heterodyne techniques.…”

Section: Introductionmentioning

confidence: 99%

Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses

et al. 2020

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Noncollinear wave-mixing spectroscopies with attosecond extreme ultraviolet (XUV) pulses provide unprecedented insight into electronic dynamics. In infrared and visible regimes, heterodyne detection techniques utilize a reference field to amplify wave-mixing signals while simultaneously allowing for phase-sensitive measurements. Here, we implement a self-heterodyned detection scheme in noncollinear wave-mixing measurements with a short attosecond XUV pulse train and two few-cycle near infrared (NIR) pulses. The initial spatiotemporally overlapped XUV and NIR pulses generate a coherence of both odd (1snp) and even (1sns and 1snd) parity states within gaseous helium. A variably delayed noncollinear NIR pulse generates angularly-dependent four-wave mixing signals that report on the evolution of this coherence. The diffuse angular structure of the XUV harmonics underlying these emission signals is used as a reference field for heterodyne detection, leading to cycle oscillations in the transient wave-mixing spectra.With this detection scheme, wave-mixing signals emitting from at least eight distinct light-induced, or dressed, states can be observed, in contrast to only one light induced state identified in a similar homodyne wave-mixing measurement. In conjunction with the self-heterodyned detection scheme, the noncollinear geometry permits the conclusive identification and angular separation of distinct wave-mixing pathways, reducing the complexity of transient spectra. These results demonstrate that the application of heterodyne detection schemes can provide signal amplification and phase-sensitivity, while maintaining the versatility and selectivity of noncollinear attosecond XUV wave-mixing spectroscopies. These techniques will be important tools in the study of ultrafast dynamics within complex chemical systems in the XUV regime.

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“…Over the last two decades, ultrashort extreme ultraviolet (XUV) pulses created through highharmonic generation (HHG) have powered the development of spectroscopic techniques which have enabled the study of atomic and molecular dynamics with femtosecond to attosecond temporal resolution. These techniques include ultrafast photoelectron and photoion spectroscopies [1][2][3][4], attosecond and femtosecond XUV transient absorption spectroscopy [5][6][7], and four-wave mixing spectroscopy [8][9][10].…”

Section: Introductionmentioning

confidence: 99%

Tunable high-order frequency mixing for XUV transient absorption and photoelectron spectroscopies

2019

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We generate tunable extreme ultraviolet emission through high-order frequency mixing between a strong near-infrared field and a weak shortwave-infrared pulse whose wavelength can be adjusted. In this two-color driving scheme, new harmonics appear in between the singlecolor harmonics at energies which are linear combinations of photons from the two pulses. We demonstrate the utility of tunable two-color harmonics by employing them for XUV transient absorption spectroscopy and time-resolved photoelectron spectroscopy. We show that the twocolor harmonics can be used to address the dynamics associated with excited states in Helium and Oxygen which are inaccessible using single-color harmonics. Specifically, we show the ability to switch between excitation of 3p and 4p states in Helium, control of transitions to the light induced states, observe new four-wave-mixing emissions, and selectively address different principal and vibrational quantum numbers associated with Oxygen Rydberg states.

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

Abstract: We demonstrate the first multidimensional spectroscopy in the extreme ultraviolet using attosecond pulses and pulse shaping.

Cited by 43 publications

References 23 publications

Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids

Transient absorption spectroscopy using high harmonic generation: a review of ultrafast X-ray dynamics in molecules and solids

Self-heterodyned detection of dressed state coherences in helium by noncollinear extreme ultraviolet wave mixing with attosecond pulses

Tunable high-order frequency mixing for XUV transient absorption and photoelectron spectroscopies

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