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Register a new userAttosecond Coherent Electron Motion in Auger-Meitner Decay
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In quantum systems, coherent superpositions of electronic states evolve on ultrafast timescales (few femtosecond to attosecond, 1 as = 0.001 fs = 10^{-18} s), leading to a time dependent charge density. Here we exploit the first attosecond soft x-ray pulses produced by an x-ray free-electron laser to induce a coherent core-hole excitation in nitric oxide. Using an additional circularly polarized infrared laser pulse we create a clock to time-resolve the electron dynamics, and demonstrate control of the coherent electron motion by tuning the photon energy of the x-ray pulse. Core-excited states offer a fundamental test bed for studying coherent electron dynamics in highly excited and strongly correlated matter.
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We present the first investigation of excited state dynamics by resonant Auger-Meitner spectroscopy (also known as resonant Auger spectroscopy) using the nucleobase thymine as an example. Thymine is photoexcited in the UV and probed with X-ray photon energies at and below the oxygen K-edge. After initial photoexcitation to a {pi}{pi}* excited state, thymine is known to undergo internal conversion to an n{pi}* excited state with a strong resonance at the oxygen K-edge, red-shifted from the ground state {pi}* resonances of thymine (see our previous study Wolf et al., Nat. Commun., 2017, 8, 29). We resolve and compare the Auger-Meitner electron spectra associated both with the excited state and ground state resonances, and distinguish participator and spectator decay contributions. Furthermore, we observe simultaneously with the decay of the n{pi}* state signatures the appearance of additional resonant Auger-Meitner contributions at photon energies between the n{pi}* state and the ground state resonances. We assign these contributions to population transfer from the n{pi}* state to a {pi}{pi}* triplet state via intersystem crossing on the picosecond timescale based on simulations of the X-ray absorption spectra in the vibrationally hot triplet state. Moreover, we identify signatures from the initially excited {pi}{pi}* singlet state which we have not observed in our previous study.
We identified interatomic Coulombic decay (ICD) channels in argon dimers after spectator-type resonant Auger decay $2p^{-1}~3d to 3p^{-2}3d, 4d$ in one of the atoms, using momentum resolved electron-ion-ion coincidence. The results illustrate that the resonant core excitation is a very efficient way of producing slow electrons at a specific site, which may cause localized radiation damage. We find also that ICD rate for $3p^{-2}4d$ is significantly lower than that for $3p^{-2}3d$.
Laser pulses with stable electric field waveforms establish the opportunity to achieve coherent control on attosecond timescales. We present experimental and theoretical results on the steering of electronic motion in a multi-electron system. A very high degree of light-waveform control over the directional emission of C+ and O+ fragments from the dissociative ionization of CO was observed. Ab initio based model calculations reveal contributions to the control related to the ionization and laser-induced population transfer between excited electronic states of CO+ during dissociation.
We demonstrate a compact technique to compress electron pulses to attosecond length, while keeping the energy spread reasonably small. The technique is based on Dielectric Laser Acceleration (DLA) in nanophotonic silicon structures. Unlike previous ballistic optical microbunching demonstrations, we use a modulator-demodulator scheme to compress phase space in the time and energy coordinates. With a second stage, we show that these pulses can be coherently accelerated, producing a net energy gain of $1.5pm0.1$ keV, which is significantly larger than the remaining energy spread of $0.88 ,_{-0.2}^{+0.0}$ keV FWHM. We show that by linearly sweeping the phase between the two stages, the energy spectrum can be coherently moved in a periodic manner, while keeping the energy spread roughly constant. After leaving the buncher, the electron pulse is also transversely focused, and can be matched into a following accelerator lattice. Thus, this setup is the prototype injector into a scalable DLA based on Alternating Phase Focusing (APF).
Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry an additional phase information, which can be retrieved by the streaking technique. In this contribution we extend the streaking formalism to include coupled electron and nuclear dynamics in molecules as well as initial coherences and demonstrate how it offers a novel tool to monitor non-adiabatic dynamics as it occurs in the vicinity of conical intersections and avoided crossings. Streaking can enhance the time resolution and provide direct signatures of electronic coherences, which affect many primary photochemical and biological events.
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