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The electro-optical properties of most semiconductors and insulators of technological interest are dominated by the presence of electron-hole quasi-particles, called excitons. The manipulation of excitons in dielectrics has recently received great attention, with possible applications in different fields including optoelectronics and photonics. Here, we apply attosecond transient reflection spectroscopy in a sequential two-foci geometry and observe sub-femtosecond dynamics of a core-level exciton in bulk MgF2 single crystals. Furthermore, we access absolute phase delays, which allow for an unambiguous comparison with theoretical calculations. Our results show that excitons surprisingly exhibit a dual atomic- and solid-like character, which manifests itself on different time scales. While the former is responsible for a femtosecond optical Stark effect, the latter dominates the attosecond excitonic response. Further theoretical investigation reveals a link with the exciton sub-femtosecond nanometric motion and allows us to envision a new route to control exciton dynamics in the close-to-petahertz regime., The capability to follow electron motion in solids is necessary to explore the ultimate speed limits of optical charge manipulation and signal processing in optoelectronic devices. Here, the authors reveal the sub-femtosecond dynamics of core excitons in MgF2 and find the dual atomic-solid nature of the exciton quasi-particle to deeply affect its ultrafast dynamics.

This is the author’s version of the work. It is posted here by permission of the AAAS for personal use, not for redistribution. The definitive version was published in Science on 354, 11 november 2016, DOI: 10.1126/science.aah5188, The dynamics of quantum systems are encoded in the amplitude and phase of wave packets. However, the rapidity of electron dynamics on the attosecond scale has precluded the complete characterization of electron wave packets in the time domain. Using spectrally resolved electron interferometry, we were able to measure the amplitude and phase of a photoelectron wave packet created through a Fano autoionizing resonance in helium. In our setup, replicas obtained by two-photon transitions interfere with reference wave packets that are formed through smooth continua, allowing the full temporal reconstruction, purely from experimental data, of the resonant wave packet released in the continuum. In turn, this resolves the buildup of the autoionizing resonance on an attosecond time scale. Our results, in excellent agreement with ab initio time-dependent calculations, raise prospects for detailed investigations of ultrafast photoemission dynamics governed by electron correlation, as well as coherent control over structured electron wave packets, We thank S. Weber for crucial contributions to the PLFA attosecond beamline, D. Cubaynes, M. Meyer, F. Penent, J. Palaudoux, for setup and test of the electron spectrometer, and O. Smirnova, for fruitful discussions. Supported by ITN-MEDEA 641789, ANR-15-CE30-0001-01-CIMBAAD, ANR11-EQPX0005-ATTOLAB, the European Research Council Advanced Grant XCHEM no. 290853, the European COST Action XLIC CM1204, and the MINECO Project no. FIS2013-42002-R. We acknowledge allocation of computer time from CCC-UAM and Mare Nostrum BSC

The ultrafast decay of highly excited electronic states is resolved with a molecular clock technique, using the vibrational motion associated to the ionic bound states as a time-reference. We demonstrate the validity of the method in the context of autoionization of the hydrogen molecule, where nearly exact full dimensional ab-initio calculations are available. The vibrationally resolved photoionization spectrum provides a time-energy mapping of the autoionization process into the bound states that is used to fully reconstruct the decay in time. A resolution of a fraction of the vibrational period is achieved. Since no assumptions are made on the underlying coupled electron-nuclear dynamics, the reconstruction procedure can be applied to describe the general problem of the decay of highly excited states in other molecular targets, We acknowledge the financial support from the FP7 Marie Curie ITN CORINF, the European Research Council under the ERC grant 290853 XCHEM, the European COST Action CM1204 XLIC and the MINECO Project No. FIS201342002-R. AP acknowledges Ramón y Cajal Programme from MINECO (Spain). LM acknowledges support from DFG priority programme 1840 QUTIF. Theoretical calculations were obtained at the Mare Nostrum BSC and CCC-UAM computer centers

Journal of Physics B: Atomic, Molecular and Optical Physics, 47 (12), ISSN:1361-6455, ISSN:0368-3508, ISSN:0953-4075, ISSN:0022-3700

Molecular absorption and photoelectron spectra can be efficiently predicted with real-time time-dependent density functional theory. We show herein how these techniques can be easily extended to study time-resolved pump-probe experiments, in which a system response (absorption or electron emission) to a probe pulse is measured in an excited state. This simulation tool helps with the interpretation of fast-evolving attosecond time-resolved spectroscopic experiments, in which electronic motion must be followed at its natural timescale. We show how the extra degrees of freedom (pump-pulse duration, intensity, frequency, and time delay), which are absent in a conventional steady-state experiment, provide additional information about electronic structure and dynamics that improve characterization of a system. As an extension of this approach, time-dependent 2D spectroscopy can also be simulated, in principle, for large-scale structures and extended systems. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim., Funded by: European Research Council. Grant Numbers: ERC-2010-AdG-Proposal No. 267374, FIS2011-65702-C02-01, PIB2010US-00652; ACI. Grant Number: ACI2009-1036; Gobierno Vasco. Grant Number: IT-319-07; European Commission. Grant Numbers: 280879-2 CRONOS CP-FP7, FP7-NMP-2008-SMALL-2, 228539; CAPES Foundation and Ministry of Education of Brazil. Grant Number: 2287/110.

We present an analytical model based on the time-dependent WKB approximation to reproduce the photoionization spectra of an H2 molecule in the autoionization region. We explore the nondissociative channel, which is the major contribution after one-photon absorption, and we focus on the features arising in the energy differential spectra due to the interference between the direct and the autoionization pathways. These features depend on both the timescale of the electronic decay of the autoionizing state and the time evolution of the vibrational wavepacket created in this state. With full ab initio calculations and with a one-dimensional approach that only takes into account the nuclear wavepacket associated to the few relevant electronic states we compare the ground state, the autoionizing state, and the background continuum electronic states. Finally, we illustrate how these features transform from molecular-like to atomic-like by increasing the mass of the system, thus making the electronic decay time shorter than the nuclear wavepacket motion associated with the resonant state. In other words, autoionization then occurs faster than the molecular dissociation into neutrals, We acknowledge computer time from the CCC-UAM and Mare Nostrum supercomputer centers and financial support by the European Research Council under the ERC Advanced Grant no. 290853 XCHEM, FP7 Marie Curie ITN CORINF, FP7 Marie Curie IRG ATTOTREND, the Ministerio de Economía y Competitividad projects FIS2010-15127, FIS2013-42002 R and ERA-Chemistry PIM2010EEC-00751, the European COST Action CM1204 XLIC, and EPSRC programme no. EP/I032517/1

The few-cycle femtosecond laser pulse has proved itself to be a powerful tool for controlling the electron dynamics inside atoms and molecules. By applying such few-cycle pulses as a driving field, single isolated attosecond pulses can be produced through the high-order harmonic generation process, which provide a novel tool for capturing the real time electron motion. The first part of the thesis is devoted to the state of the art few-cycle near infrared (NIR) laser pulse development, which includes absolute phase control (carrier-envelope phase stabilization), amplitude control (power stabilization), and relative phase control (pulse compression and shaping). Then the double optical gating (DOG) method for generating single attosecond pulses and the attosecond streaking experiment for characterizing such pulses are presented. Various experimental limitations in the attosecond streaking measurement are illustrated through simulation. Finally by using the single attosecond pulses generated by DOG, an attosecond transient absorption experiment is performed to study the autoionization process of argon. When the delay between a few-cycle NIR pulse and a single attosecond XUV pulse is scanned, the Fano resonance shapes of the argon autoionizing states are modified by the NIR pulse, which shows the direct observation and control of electron-electron correlation in the temporal domain.