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Metasurfaces are arrays of subwavelength spaced nanostructures that can manipulate the amplitude, phase, and polarization of light to achieve a variety of optical functions beyond the capabilities of 3D bulk optics. However, they suffer from limited performance and efficiency when multiple functions with large deflection angles are required because the non-local interactions due to optical coupling between nanostructures are not fully considered. Here we introduce a method based on supercell metasurfaces to demonstrate multiple independent optical functions at arbitrary large deflection angles with high efficiency. In one implementation the incident laser is simultaneously diffracted into Gaussian, helical and Bessel beams over a large angular range. We then demonstrate a compact wavelength-tunable external cavity laser with arbitrary beam control capabilities – including beam shaping operations and the generation of freeform holograms. Our approach paves the way to novel methods to engineer the emission of optical sources., The angular dependence is a well-known issue in metasurface engineering. Here the authors introduce a supercell metasurface able to implement multiple independent functions under large deflection angles with high efficiency, leading to a wavelength tunable laser with arbitrary wavefront control.

We report measurements of the temporal dynamics of the valence band photoemission from the magnesium (0001) surface across the resonance of the Γ surface state at 134 eV and link them to observations of high-resolution synchrotron photoemission and numerical calculations of the time-dependent Schrödinger equation using an effective single-electron model potential. We observe a decrease in the time delay between photoemission from delocalized valence states and the localized core orbitals on resonance. Our approach to rigorously link excitation energy-resolved conventional steady-state photoemission with attosecond streaking spectroscopy reveals the connection between energy-space properties of bound electronic states and the temporal dynamics of the fundamental electronic excitations underlying the photoelectric effect., We thank F. Siegrist for experimental assistance, and we acknowledge financial support by the Munich Centre for Advanced Photonics (MAP). R. K. acknowledges an ERC Consolidator Grant “AEDMOS” (ERC-2014-CoG AEDMOS). D. P. acknowledges support from the “MEDEA” (H2020- MSCA-ITN-2014-641789-MEDEA).

Photodissociation of ozone following absorption of biologically harmful solar ultraviolet radiation is the key mechanism for the life protecting properties of the atmospheric ozone layer. Even though ozone photolysis is described successfully by post-Hartree-Fock theory, it has evaded direct experimental access so far, due to the unavailability of intense ultrashort deep ultraviolet radiation sources. The rapidity of ozone photolysis with predicted values of a few tens of femtoseconds renders both ultrashort pump and probe pulses indispensable to capture this manifestation of ultrafast chemistry. Here, we present the observation of femtosecond time-scale electronic and nuclear dynamics of ozone triggered by \ensuremath{\sim}10-fs, \ensuremath{\sim}2-\textmu{}J deep ultraviolet pulses and, in contrast to conventional attochemistry experiments, probed by extreme ultraviolet isolated pulses. An electronic wave packet is first created. We follow the splitting of the excited B-state related nuclear wave packet into a path leading to molecular fragmentation and an oscillating path, revolving around the Franck-Condon point with 22-fs wave-packet revival time. Full quantum-mechanical ab initio multiconfigurational time-dependent Hartree simulations support this interpretation.

Physical review / A covering atomic, molecular, and optical physics and quantum information 100(5), 053420 (2019). doi:10.1103/PhysRevA.100.053420, Highly brilliant, coherent, femtosecond x-ray pulses delivered by free-electron lasers (FELs) constitute oneof the pillars of modern ultrafast science. Next generation FEL facilities provide up to megahertz repetitionrates and pulse durations down to the attosecond regime utilizing self-amplification of spontaneous emission.However, the stochastic nature of this generation mechanism demands single-shot pulse characterization toperform meaningful experiments. Here we demonstrate a fast yet robust online analysis technique capableof megahertz-rate mapping of the temporal intensity structure and arrival time of x-ray FEL pulses withfew-femtosecond resolution. We performed angular streaking measurements of both neon photo- and Augerelectrons and show their applicability for a direct time-domain feedback system during ongoing experiments.The fidelity of the real-time pulse characterization algorithm is corroborated by resolving isolated x-ray pulsesand double pulse trains with few-femtosecond substructure, thus paving the way for x-ray-pump–x-ray-probeFEL science at repetition rates compatible with the demands of LCLS-II and European XFEL., Published by Inst., Woodbury, NY

Photoemission of an electron is commonly treated as a one-particle phenomenon. With attosecond streaking spectroscopy we observe the breakdown of this single active-electron approximation by recording up to six attoseconds retardation of the dislodged photoelectron due to electronic correlations. We recorded the photon-energy-dependent emission timing of electrons, released from the helium ground state by an extreme-ultraviolet photon, either leaving the ion in its ground state or exciting it into a shake-up state. We identify an optical field-driven d.c. Stark shift of charge-asymmetric ionic states formed after the entangled photoemission as a key contribution to the observed correlation time shift. These findings enable a complete wavepacket reconstruction and are universal for all polarized initial and final states. Sub-attosecond agreement with quantum mechanical ab initio modelling allows us to determine the absolute zero of time in the photoelectric effect to a precision better than 1/25th of the atomic unit of time. Photoemission is not a simple process and it is not instantaneous. Delays of a few attoseconds have now been measured in helium and it seems that they are partly due to electronic correlations.

Photoemission spectroscopy is central to understanding the inner workings of condensed matter, from simple metals and semiconductors to complex materials such as Mott insulators and superconductors1. Most state-of-the-art knowledge about such solids stems from spectroscopic investigations, and use of subfemtosecond light pulses can provide a time-domain perspective. For example, attosecond (10-18 seconds) metrology allows electron wave packet creation, transport and scattering to be followed on atomic length scales and on attosecond timescales2-7. However, previous studies could not disclose the duration of these processes, because the arrival time of the photons was not known with attosecond precision. Here we show that this main source of ambiguity can be overcome by introducing the atomic chronoscope method, which references all measured timings to the moment of light-pulse arrival and therefore provides absolute timing of the processes under scrutiny. Our proof-of-principle experiment reveals that photoemission from the tungsten conduction band can proceed faster than previously anticipated. By contrast, the duration of electron emanation from core states is correctly described by semiclassical modelling. These findings highlight the necessity of treating the origin, initial excitation and transport of electrons in advanced modelling of the attosecond response of solids, and our absolute data provide a benchmark. Starting from a robustly characterized surface, we then extend attosecond spectroscopy towards isolating the emission properties of atomic adsorbates on surfaces and demonstrate that these act as photoemitters with instantaneous response. We also find that the tungsten core-electron timing remains unchanged by the adsorption of less than one monolayer of dielectric atoms, providing a starting point for the exploration of excitation and charge migration in technologically and biologically relevant adsorbate systems.