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We demonstrate the ability to control and shape the spectrotemporal content of extreme-ultraviolet (XUV) pulses produced by a seeded free-electron laser (FEL). The control over the spectrotemporal properties of XUV light was achieved by precisely manipulating the linear frequency chirp of the seed laser. Our results agree with existing theory, which allows us to retrieve the temporal properties (amplitude and phase) of the FEL pulse from measurements of the spectra as a function of the FEL operating parameters. Furthermore, we show the first direct evidence of the full temporal coherence of FEL light and generate Fourier limited pulses by fine-tuning the FEL temporal phase. The possibility of tailoring the spectrotemporal content of intense short-wavelength pulses represents the first step towards efficient nonlinear optics in the XUV to x-ray spectral region and will enable precise manipulation of core-electron excitations using the methods of coherent quantum control. [ABSTRACT FROM AUTHOR]

In a coherent control experiment, light pulses are used to guide the real-time evolution of a quantum system. This requires the coherence and the control of the pulses' electric-field carrier waves. In this work, we use frequency-domain interferometry to demonstrate the mutual coherence of time-delayed pulses generated by an extreme ultraviolet seeded free-electron laser. Furthermore, we use the driving seed laser to lock and precisely control the relative phase between the two free-electron laser pulses. This new capability opens the way to a multitude of coherent control experiments, which will take advantage of the high intensity, short wavelength, and short duration of the pulses generated by seeded free-electron lasers. [ABSTRACT FROM AUTHOR]

We demonstrate the generation of extreme-ultraviolet (XUV) free-electron laser (FEL) pulses with time-dependent polarization. To achieve polarization modulation on a femtosecond timescale, we combine two mutually delayed counterrotating circularly polarized subpulses from two cross-polarized undulators. The polarization profile of the pulses is probed by angle-resolved photoemission and above-threshold ionization of helium; the results agree with solutions of the time-dependent Schrödinger equation. The stability limit of the scheme is mainly set by electron-beam energy fluctuations, however, at a level that will not compromise experiments in the XUV. Our results demonstrate the potential to improve the resolution and element selectivity of methods based on polarization shaping and may lead to the development of new coherent control schemes for probing and manipulating core electrons in matter.

Triggering and switching magnetic moments is of key importance for applications ranging from spintronics to quantum information. A noninvasive ultrafast control at the nanoscale is, however, an open challenge. Here, we propose a novel laser-based scheme for generating atomic-scale charge current loops within femtoseconds. The associated orbital magnetic moments remain ferromagnetically aligned after the laser pulses have ceased and are localized within an area that is tunable via laser parameters and can be chosen to be well below the diffraction limit of the driving laser field. The scheme relies on tuning the phase, polarization, and intensities of two copropagating Gaussian and vortex laser pulses, allowing us to control the spatial extent, direction, and strength of the atomic-scale charge current loops induced in the irradiated sample upon photon absorption. In the experiment we used He atoms driven by an ultraviolet and infrared vortex-beam laser pulses to generate current-carrying Rydberg states and test for the generated magnetic moments via dichroic effects in photoemission. Ab initio quantum dynamic simulations and analysis confirm the proposed scenario and provide a quantitative estimate of the generated local moments.