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Attosecond Spectroscopy of Liquid Water Rounding Gas Phase

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Attosecond Spectroscopy of Liquid Water Rounding Gas Phase RESEARCH CHEMICAL PHYSICS quartz nozzle with an inner diameter of ~25 mm. Evaporation from the jet created the sur- Attosecond spectroscopy of liquid water rounding gas phase. An extreme ultraviolet (XUV) attosecond pulse train (APT), obtained Inga Jordan, Martin Huppert*, Dominik Rattenbacher†, Michael Peper, Denis Jelovina, Conaill Perry, through high-harmonic generation of a ~30-fs Aaron von Conta, Axel Schild, Hans Jakob Wörner‡ near-IR laser pulse in an argon gas cell, was focused onto the liquid microjet (spot size Electronic dynamics in liquids are of fundamental importance, but time-resolved experiments have so far ~50 mm) together with a strongly attenuated remained limited to the femtosecond time scale. We report the extension of attosecond spectroscopy to the replica of the IR laser pulse. This resulted in liquid phase. We measured time delays of 50 to 70 attoseconds between the photoemission from liquid water the detection of electrons from both phases and that from gaseous water at photon energies of 21.7 to 31.0 electron volts. These photoemission delays simultaneously. [See (31) for details of the can be decomposed into a photoionization delay sensitive to the local environment and a delay originating from experimental setup.] electron transport. In our experiments, the latter contribution is shown to be negligible. By referencing liquid The photoelectron signals from the liquid water to gaseous water, we isolated the effect of solvation on the attosecond photoionization dynamics of phase were shifted and broadened relative to water molecules. Our methods define an approach to separating bound and unbound electron dynamics from the gas-phase signals, which enabled their dis- the structural response of the solvent. crimination. Photoemission induced by the APT created several replicas of the photo- electron spectra (Fig. 1, blue). The simulta- he study of liquid water has been at the with attosecond temporal resolutions (14–17), neous presence of the APT and IR pulses heart of physical sciences since their a deeper understanding of electronic dynamics resulted in the formation of sideband spec- Downloaded from emergence. Although undoubtedly the in real chemical and biological processes re- tra (Fig. 1, red). Because these sidebands can T most studied liquid, water has proper- quires an extension of attosecond science to be created through two different quantum ties that are still not entirely understood. the liquid phase. As the main distinguishing pathways, their intensity oscillates as a func- Water displays more than 70 anomalies in its feature relative to most femtosecond spectros- tion of the delay between the APT and IR physical properties (1–3), such as density, heat copies, the inherent time scale of the present pulses. capacity, or thermal conductivity. Even the measurements freezes all types of structural A general challenge in attosecond time- structure of liquid water with its rapidly fluc- dynamics, leaving only the fastest electronic resolved measurements originates from the http://science.sciencemag.org/ tuating hydrogen-bond network remains an dynamics as possible contributions. spectral bandwidth of attosecond pulses. The object of intense debate (4–7). Many open We concentrated on the measurement of resulting spectral congestion is considerably questions are associated with liquid water, time delays in photoemission. Previous mea- reduced by using an APT (17, 32). Nonetheless, and their far-reaching implications explain surements on atoms (18, 19) and molecules most complex systems usually have broad the considerable attention that it has always (17, 20), with supporting theoretical work photoelectron spectra, which makes the ap- attracted. A wide variety of experimental tech- (21–23), established that such experiments plication of attosecond photoelectron spec- niques have therefore been applied to its study, access photoionization delays caused by the troscopy difficult. This challenge has been including nuclear magnetic resonance (8), in- propagation of the photoelectron through the addressed by using metallic filters to reduce frared (IR) spectroscopy (9), x-ray spectros- potential created by the parent ion. Similar the spectral overlap (17, 19) and additionally copies (10), and x-ray scattering (11). measurements on metals (24–26) revealed the performing an energy-dependent analysis of on August 24, 2020 Despite these considerable efforts, many dominant influence of the electron transport the sideband oscillation phases (32, 33). In properties of liquid water remain mysterious. time from the point of ionization to the sur- the general case of broad overlapping photo- This fact is partially the consequence of a face. The additional role of initial-state and electron spectra, these approaches are no longer mismatch between the temporal resolution final-state effects was highlighted in (27–29). sufficient. We therefore combined these ideas of the available techniques and the ultrafast Recent work on nanoparticles (30) interpreted with a general approach: the complex-valued dynamics of liquid water. A prominent ex- the time delays as being dominantly sensitive principal components analysis (CVPCA) that ample is the observation of a splitting in the to inelastic scattering times on the basis of was numerically validated in (34). x-ray emission spectrum of the outermost va- purely classical simulations that neglected the Figure 2 shows the experimental results ob- lence band of liquid water, which is assigned time delays due to photoionization and scat- tained with APTs transmitted through Sn or either to two structural motifs of liquid water, tering. Here, we developed a model that de- Ti filters, respectively, resulting in a spectral differing in their hydrogen-bond structure scribes such time delays on a fully quantum restriction to harmonic orders 11, 13, and (12), or to dynamics in the core-hole state (13). mechanical level and combined it with a 15 (Sn) or 17, 19, and 21 (Ti). Shown in Fig. 2, A Differentiation of these two interpretations would semiclassical-trajectory Monte Carlo simula- and B, are the photoelectron spectra recorded require subfemtosecond temporal resolution. tion of electron transport, which includes in the absence (blue circles) or presence (orange Hence, probing liquid water on ever shorter elastic and inelastic electron scattering, the circles) of the IR field; Fig. 2, C and D, shows time scales may allow for a better understand- quantum mechanical phase accumulated along the difference spectrum (“IR on”–“IR off”; ingofatleastsomeofits unusual properties. all possible electron trajectories, and the re- black circles) recorded on a single-shot basis Here, we used attosecond spectroscopy to sulting interference effects. We show that, in by chopping the IR beam at half of the laser study liquid water. Whereas isolated molecules general, the measured time delays encode both repetition rate. The spectra are dominated of increasing complexity have been studied scattering delays and mean free paths in ad- by the photoelectrons originating from the dition to the photoemission delay. highest valence band of liquid water (light The concept of our measurement is illus- blue), the highest occupied molecular orbital Laboratorium für Physikalische Chemie, ETH Zürich, Zürich, trated in Fig. 1. We used attosecond interfer- (HOMO) of isolated water molecules (dark Switzerland. ometry to measure the time delay between the blue), and the respective sidebands (light *Present address: Paul Scherrer Institut, CH-5232 Villigen PSI, photoemission from liquid water and that and dark orange, respectively). Switzerland. †Present address: Max Planck Institute for the Science of Light, D-91058 Erlangen, Germany. from gaseous water. Liquid water was intro- To achieve the highest accuracy, we based ‡Corresponding author. Email: [email protected] duced into a vacuum chamber through a the analysis on principal component spectra Jordan et al., Science 369, 974–979 (2020) 21 August 2020 1of6 RESEARCH | REPORT Fig. 1. Attosecond time- resolved photoelectron spectroscopy of liquid water. A spectrally filtered attosecond pulse train composed of a few high-harmonic orders (such as H(q–1) and H(q+1)), superimposed with a near-IR femtosecond laser pulse, interacts with a microjet of liquid water. Photoelectrons are simultaneously emitted from the liquid and the surrounding gas phase. The resulting photoelectron spectra are measured as a function of the time delay between the overlapping pulses. Downloaded from that were measured with the same liquid- obtain Dt = 49 ± 16 as. The statistical analyses the laser-assisted photoelectric effect (LAPE) microjet photoelectron spectrometer (35), but leading to these results are given in table S1 with laser-assisted electron scattering (LAES). replacing the APT with isolated high-order and figs. S4 and S5 (31). The positive sign of We distinguish “local” pathways, when the harmonics selected in a time-preserving mono- the relative delays indicates that the electrons XUV and IR fields act at the same location chromator (36). [See (31) and fig. S1 for the from liquid water appear to be emitted later in space, from “nonlocal” pathways where http://science.sciencemag.org/ corresponding photoelectron spectra obtained than those from water vapor. the XUV interaction (photoionization) and with harmonics 11 to 21.] These principal com- The modulation depth M,whereM =1sig- IR interaction (LAES) take place at differ- ponents were used to decompose the photo- nifies a perfect
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