Coherent interaction of femtosecond extreme-uv light with He atoms

Strasser, Daniel; Pfeifer, Thomas; Hom, Brian J.; Müller, Astrid M.; Plenge, J.; Leone, Stephen R.

doi:10.1103/physreva.73.021805

Cited by 29 publications

(31 citation statements)

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“…It has been shown in recent studies that the photon energy range can be considerably extended into the water window of several 100 eV and beyond (34)(35)(36)(37)(38)(39)(40) but applications with these sources up to now are scarce. For ultrafast applications, time-resolved photoelectron spectroscopy (PES) (41) with pump-probe schemes where the sample is pumped with a laser pulse and probed with HHG pulses at a defined pump-probe delay has emerged as a powerful tool for the investigation of ultrafast dynamics in gas phase samples (42)(43)(44)(45)(46)(47) and on surfaces (48)(49)(50)(51)(52)(53)(54). A variety of set ups has been described to perform such experiments on gas phase samples (55)(56)(57)(58)(59)(60), on surfaces (61-64) or on both (65,66).…”

Section: Introductionmentioning

confidence: 99%

Femtosecond time-resolved photoelectron spectroscopy with a vacuum-ultraviolet photon source based on laser high-order harmonic generation

Wernet

Gaudin

Godehusen

et al. 2011

Review of Scientific Instruments

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A laser-based tabletop approach to femtosecond time-resolved photoelectron spectroscopy with photons in the vacuum-ultraviolet (VUV) energy range is described. The femtosecond VUV pulses are produced by high-order harmonic generation (HHG) of an amplified femtosecond Ti:sapphire laser system. Two generations of the same set up and results from photoelectron spectroscopy in the gas phase are discussed. In both generations a toroidal grating monochromator was used to select one harmonic in the photon energy range of 20-30 eV. The first generation of the set up was used to perform photoelectron spectroscopy in the gas phase to determine the bandwidth of the source. We find that our HHG source has a bandwidth of 140±40 meV. The second and current generation is optimized for femtosecond pump-probe photoelectron spectroscopy with high flux and a small spot size at the sample of the femtosecond probe pulses. The VUV radiation is focused into the interaction region with a toroidal mirror to a spot smaller than 100 x 100 μm 2 and the flux amounts to 10 10 photons/s at the sample at a repetition rate of 1 kHz. The duration of the monochromatized VUV pulses is determined to be 120 femtoseconds resulting in an overall pump-probe time resolution of 135±5 fs. We show how this set up can be used to map the transient valence electronic structure in molecular dissociation.3

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Section: Introductionmentioning

confidence: 99%

Femtosecond time-resolved photoelectron spectroscopy with a vacuum-ultraviolet photon source based on laser high-order harmonic generation

Wernet

Gaudin

Godehusen

et al. 2011

Review of Scientific Instruments

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“…Another, more nm, 400 nm, or 266 nm photon. 6 The observed implentations of the soft x-ray pulses to In He the overlap of the two pulses, temporally harmonic. and spatially, is detected readily.…”

Section: Phase-shaping Of Soft X-ray Pulsesmentioning

confidence: 99%

“…However, some in the 12-14 eV region, which makes the results very preliminary. Investigations have also been initiated on W(CO) 6 (Fig. 3).…”

Section: Photoelectron Angular Imaging Of Rydberg Wave Packetsmentioning

confidence: 99%

“…The advantages of this system are the ability to collect a large solid angle of the emitted electrons and the elimination of stray electron signals by confining the zone of collection to a very small region around the high field magnets. Figure 3 shows an example of a photoelectron spectrum of a complex molecule, W(CO) 6 . The intrinsic resolution of this magnetic bottle is measured to be AE/E of 4%.24…”

Section: _0mentioning

confidence: 99%

“…Core level spectroscopy of AIBr 3 versus Al 2 Br 6 In preparation for pump-probe experiments on aluminum bromide species, a series of experiments were performed to obtain the valence and core level photoelectron spectra of AIBr 3 and its dimer A1 2 Br 6 at the Advanced Light Source. "…”

Section: 5-bridgingmentioning

confidence: 99%

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Ultrafast Soft X-Ray Probing of Core Level Molecular Dynamics

Leone¹

2006

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Public reporting; burden for tI~s collection of information is estimated to &verg o rperesponse, incldingdou h time for revievAning~structions, seareN nge istn data sources, athering and maintaining fth data needed, and completing an revawin thiscolaection of information.= Sen co rent garding Nos bken estimate or any o" aspeclt of hi cot ci no information.,r rigcu .u~atoi frrdun this burden to Department of Defense, Wasilington Headquarters Services, tDreclorate for tinformation operatiors anid AFRL-SR-AR-TR-07-O061Approved for Public Release; distribution is unlimited. SUPPLEMENTARY NOTES ABSTRACTThis research program explored time-resolved dynamics of molecular systems by femtosecond photoelectron spectroscopy using high order harmonics. Ultrafast soft x-ray laser pump/probe studies revealed changes in binding relations and atomic core level shifts in the molecules during chemical rearrangements by detecting the changes in photoelectron energies as a function of internuclear separation in dissociative states in real time.Harmonic pulses with photon energies up to 100 eV and femtosecond time resolution were produced with excellent efficiency and pulse-to-pulse stability.Valence and core photoelectron spectra were obtained on neutral atoms and molecules.Phase manipulation of high order harmonics was achieved.Photoelectron spectra and photoionization mass spectra of gas phase ionic liquids were obtained. Two color excitation spectra of bromine molecules were investigated, as well as Rydberg wave packet photoelectron angular distributions.Pump/probe experiments on the photodissociation of metal carbonyls, halogens, and aluminum halides were also under investigation. Executive Summary This research program explores the time-resolved reaction and fragmentation dynamics of diatomic and polyatomic molecules using femtosecond valence and core level photoelectron spectroscopy."' The chemical shifts in the electron energies provide direct information about the changes in electron orbital configurations as a function of internuclear separation in dissociative states of these molecules. Ultrafast soft x-ray laser pump/probe experiments take advantage of the femtosecond time resolution capability of a novel high order harmonic x-ray source by detecting time resolved valence electrons and atomic core level shifts in excited species as well as changes in the photo-ion mass distribution during chemical rearrangements. The experiments probe time-resolved valence (PES) and core level (XPS) spectroscopies on excited states and during photofragmentation of simple diatomics, metal halogen, and carbonyl species, as well as intramolecular processes in polyatomic molecules. The apparatus produces high order harmonics of a Ti:sapphire laser in the x-ray region of the spectrum with ultrafast pulse durations and is used to measure valence orbitals and atomic core levels during reactions and dissociation. The instrument consists of a 2.5 mJ pulse energy, 1000 Hz repetition rate Ti:sapphire laser system, a 1000 Hz pulsed jet of rare gas ...

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Two pathways and an isotope effect in H3+ formation following double ionization of methanol

et al. 2021

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The trihydrogen ion has a central role in creating complex molecules in the interstellar medium. Therefore, its formation and destruction mechanisms in high photon energy environments involving organic molecules are drawing significant experimental and theoretical attention. Here, we employ a combination of time‐resolved ultrafast extreme‐ultraviolet pump and near‐infrared probe spectroscopy applied to the deuterated CH3OD methanol molecule. Similar to other double‐ionization studies, the isotopic labeling reveals two competing pathways for forming trihydrogen: A) normalH3++COnormalH+ and B) normalH3++HCnormalO+. We validate our high‐level ab initio nonadiabatic molecular dynamic simulations by showing that it closely reproduces the essential features of the measured kinetic energy release distribution and branching ratios of the two pathways of the deuterated system. The success of ab initio simulation in describing single photon double‐ionization allows for an unprecedented peek into the formation pathways for the undeuterated species, beyond present experimental reach. For this case, we find that the kinetic energy release of pathway B shifts to lower energies by more than 0.6 eV due to a dynamical isotope effect. We also determine the mechanism for trihydrogen formation from excited states of the dication and elucidate the isotope effect's role in the observed dynamics.

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Coherent interaction of femtosecond extreme-uv light with He atoms

Cited by 29 publications

References 25 publications

Femtosecond time-resolved photoelectron spectroscopy with a vacuum-ultraviolet photon source based on laser high-order harmonic generation

Femtosecond time-resolved photoelectron spectroscopy with a vacuum-ultraviolet photon source based on laser high-order harmonic generation

Ultrafast Soft X-Ray Probing of Core Level Molecular Dynamics

Two pathways and an isotope effect in H3+ formation following double ionization of methanol

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