Angular dependence of photoemission time delay in helium

Abstract

Time delays of electrons emitted from an isotropic initial state with the absorption of a single photon and leaving behind an isotropic ion are angle independent. Using an interferometric method involving XUV attosecond pulse trains and an IR-probe field in combination with a detection scheme, which allows for full three-dimensional momentum resolution, we show that measured time delays between electrons liberated from the 1s2 spherically symmetric ground state of helium depend on the emission direction of the electrons relative to the common linear polarization axis of the ionizing XUV light and the IR-probing field. Such time delay anisotropy, for which we measure values as large as 60 as, is caused by the interplay between final quantum states with different symmetry and arises naturally whenever the photoionization process involves the exchange of more than one photon. With the support of accurate theoretical models, the angular dependence of the time delay is attributed to small phase differences that are induced in the laser-driven continuum transitions to the final states. Since most measurement techniques tracing attosecond electron dynamics involve the exchange of at least two photons, this is a general and significant effect that must be taken into account in all measurements of time delays involving photoionization processes ; S.H, C.C, L.G., and U.K. acknowledge support by the ERC advanced Grant No. ERC-2012-ADG_20120216 within the seventh framework program of the European Union and by the NCCR MUST, funded by the Swiss National Science Foundation. M.L. acknowledges support from the ETH Zurich Postdoctoral Fellowship Program. A.J.G., L.A., and F.M. acknowledge the support from the European Research Council under the ERC Grant No. 290853 XCHEM, from the European COST Action No. CM1204 XLIC, the MINECO Project No. FIS2013-42002-R, the ERA-Chemistry Project No. PIM2010EEC- 00751, and the European Grant No. MC-ITN CORINF. Calculations were performed at the Centro de Computacion Científica of the Universidad Autónoma de Madrid (CC-UAM) and the Barcelona Supercomputing Center (BSC). I.I. and A.S.K. acknowledge support of the Australian Research Council (Grant No. DP120101805) and the use of the National Computational Infrastructure Facility. J.M.D. acknowledges support from the Swedish Research Grants No. 2013-344 and No. 2014-3724. E.L. acknowledges support from the Swedish Research Council, Grant No. 2012-3668. Moreover, this research was supported in part by the Kavli Institute for Theoretical Physics (National Science Foundation under Grant No. NSF PHY11-25915) and by NORDITA, the Nordic Institute for Theoretical Physics