Communication: XUV transient absorption spectroscopy of iodomethane and iodobenzene photodissociation

Drescher, Lorenz; Galbraith, M. C. E.; Reitsma, Geert; Durá, J.; Zhavoronkov, N.; Patchkovskii, Serguei; Vrakking, Marc J. J.; Mikosch, Jochen

doi:10.1063/1.4955212

Cited by 38 publications

(42 citation statements)

References 34 publications

(25 reference statements)

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“…The experiments were carried out with a two-colour XUV-VIS/NIR pump-probe setup, which has already largely been described elsewhere 40 – 42 . The experimental apparatus was upgraded for the present study by compressing the output pulses of a 1 kHz Ti:Sa amplifier by means of a hollow-core fibre setup and a set of chirped mirrors.…”

Section: Methodsmentioning

confidence: 99%

Few-femtosecond passage of conical intersections in the benzene cation

Galbraith¹,

Scheit

Golubev

et al. 2017

Nat Commun

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Observing the crucial first few femtoseconds of photochemical reactions requires tools typically not available in the femtochemistry toolkit. Such dynamics are now within reach with the instruments provided by attosecond science. Here, we apply experimental and theoretical methods to assess the ultrafast nonadiabatic vibronic processes in a prototypical complex system—the excited benzene cation. We use few-femtosecond duration extreme ultraviolet and visible/near-infrared laser pulses to prepare and probe excited cationic states and observe two relaxation timescales of 11 ± 3 fs and 110 ± 20 fs. These are interpreted in terms of population transfer via two sequential conical intersections. The experimental results are quantitatively compared with state-of-the-art multi-configuration time-dependent Hartree calculations showing convincing agreement in the timescales. By characterising one of the fastest internal conversion processes studied to date, we enter an extreme regime of ultrafast molecular dynamics, paving the way to tracking and controlling purely electronic dynamics in complex molecules.

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Section: Methodsmentioning

confidence: 99%

Few-femtosecond passage of conical intersections in the benzene cation

Galbraith¹,

Scheit

Golubev

et al. 2017

Nat Commun

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“…It is a prototypical polyatomic quantum system whose photophysical and photochemical properties including extreme-ultraviolet-induced ionization of inner-shell electrons are well-studied424344. At a photon excitation energy of 68.6 eV (18.1 nm) the valence and inner-shell photoionization cross-sections are similar44.…”

Section: Discussionmentioning

confidence: 99%

Attosecond interferometry with self-amplified spontaneous emission of a free-electron laser

et al. 2017

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Light-phase-sensitive techniques, such as coherent multidimensional spectroscopy, are well-established in a broad spectral range, already spanning from radio-frequencies in nuclear magnetic resonance spectroscopy to visible and ultraviolet wavelengths in nonlinear optics with table-top lasers. In these cases, the ability to tailor the phases of electromagnetic waves with high precision is essential. Here we achieve phase control of extreme-ultraviolet pulses from a free-electron laser (FEL) on the attosecond timescale in a Michelson-type all-reflective interferometric autocorrelator. By varying the relative phase of the generated pulse replicas with sub-cycle precision we observe the field interference, that is, the light-wave oscillation with a period of 129 as. The successful transfer of a powerful optical method towards short-wavelength FEL science and technology paves the way towards utilization of advanced nonlinear methodologies even at partially coherent soft X-ray FEL sources that rely on self-amplified spontaneous emission.

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“…XUV prism experiments. The XUV prism experiments were performed at an HHG beamline that was previously described in detail [50][51][52]. NIR pulses with a duration of 4.5 fs were obtained by spectrally broadening the output of a commercial Ti:sapphire amplifier in a differentially pumped hollow-core fiber that was filled with Ne.…”

Section: Methodsmentioning

confidence: 99%

Extreme-ultraviolet refractive optics

Drescher¹,

Kornilov²,

Witting³

et al. 2018

Nature

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Refraction is a well-known optical phenomenon that alters the direction of light waves propagating through matter. Microscopes, lenses and prisms based on refraction are indispensable tools for controlling the properties of light beams at visible, infrared, ultraviolet and X-ray wavelengths. The large absorption of extreme-ultraviolet (XUV) radiation in matter, however, hinders the development of refractive lenses and prisms in this spectral region. Here, we demonstrate control over the refraction of XUV radiation by using a gas jet with a density gradient across the XUV beam profile. A gas phase prism is demonstrated that leads to a frequency-dependent deflection of the XUV beam. The strong deflection in the vicinity of atomic resonances is further used to develop a deformable XUV refractive lens, with low absorption and a focal length that can be tuned by varying the gas pressure. Our results provide novel opportunities in XUV science and open a route towards the transfer of refraction-based techniques including microscopy and nanofocusing, which are well established in other spectral regions, to the XUV domain.

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Communication: XUV transient absorption spectroscopy of iodomethane and iodobenzene photodissociation

Cited by 38 publications

References 34 publications

Few-femtosecond passage of conical intersections in the benzene cation

Few-femtosecond passage of conical intersections in the benzene cation

Attosecond interferometry with self-amplified spontaneous emission of a free-electron laser

Extreme-ultraviolet refractive optics

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