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Ultrafast processes in matter, such as the electron emission after light absorption, can now be studied using ultrashort light pulses of attosecond duration (10−18 seconds) in the extreme ultraviolet spectral range. The lack of spectral resolution due to the use of short light pulses has raised issues in the interpretation of the experimental results and the comparison with theoretical calculations. We determine photoionization time delays in neon atoms over a 40–electron volt energy range with an interferometric technique combining high temporal and spectral resolution. We spectrally disentangle direct ionization from ionization with shake-up, in which a second electron is left in an excited state, and obtain excellent agreement with theoretical calculations, thereby solving a puzzle raised by 7-year-old measurements.

Attosecond pulses are central to the investigation of valence- and core-electron dynamics on their natural timescales 1 – 3 . The reproducible generation and characterization of attosecond waveforms has been demonstrated so far only through the process of high-order harmonic generation 4 – 7 . Several methods for shaping attosecond waveforms have been proposed, including the use of metallic filters 8 , 9 , multilayer mirrors 10 and manipulation of the driving field 11 . However, none of these approaches allows the flexible manipulation of the temporal characteristics of the attosecond waveforms, and they suffer from the low conversion efficiency of the high-order harmonic generation process. Free-electron lasers, by contrast, deliver femtosecond, extreme-ultraviolet and X-ray pulses with energies ranging from tens of microjoules to a few millijoules 12 , 13 . Recent experiments have shown that they can generate subfemtosecond spikes, but with temporal characteristics that change shot-to-shot 14 – 16 . Here we report reproducible generation of high-energy (microjoule level) attosecond waveforms using a seeded free-electron laser 17 . We demonstrate amplitude and phase manipulation of the harmonic components of an attosecond pulse train in combination with an approach for its temporal reconstruction. The results presented here open the way to performing attosecond time-resolved experiments with free-electron lasers. Generation of intense attosecond waveforms with independently controllable amplitude and phase is performed by using a seeded free-electron laser.

Nonlinear optics is the study of the interaction of intense laser light with matter. This Third Edition has been rewritten to conform to the standard SI system of units and includes comprehensively updated material on the latest developments in the field. The book introduces the entire field of optical physics and specifically the area of nonlinear optics. It focuses on the fundamental issues including the electromagnetic origin of optical phenomena, the quantum mechanical description of the optical properties of matter, the role of spatial symmetries in determining the optical response, causality and Kramers Kronig relations, and ultrafast and high intensity optical effects.

A photoelectron, emitted due to the absorption of light quanta as described by the photoelectric effect, is often characterized experimentally by a classical quantity, its momentum. However, since the photoelectron is a quantum object, its rigorous characterization requires the reconstruction of the complete quantum state, the photoelectron’s density matrix. Here we use quantum-state tomography to fully characterize photoelectrons emitted from helium and argon atoms upon absorption of ultrashort, extreme ultraviolet light pulses. While in helium we measure a pure photoelectronic state, in argon, spin–orbit interaction induces entanglement between the ion and the photoelectron, leading to a reduced purity of the photoelectron state. Our work shows how state tomography gives new insights into the fundamental quantum aspects of light-induced electronic processes in matter, bridging the fields of photoelectron spectroscopy and quantum information and offering new spectroscopic possibilities for quantum technology. Photoelectron quantum-state tomography is demonstrated in helium and argon atoms upon the absorption of ultrashort, extreme ultraviolet light pulses. The purity and degree of entanglement of a mixed photoelectron and ion state are quantified following coherent two-photon ionization using an extreme ultraviolet pulse and two infrared pulses.

Phase matching is a critical requirement for coherent nonlinear optical processes such as frequency conversion and parametric amplification. Phase mismatch prevents microscopic nonlinear sources from combining constructively, resulting in destructive interference and thus very low efficiency. We report the experimental demonstration of phase mismatch-free nonlinear generation in a zero-index optical meta materia I. In contrast to phase mismatch compensation techniques required in conventional nonlinear media, the zero index eliminates the need for phase matching, allowing efficient nonlinear generation in both forward and backward directions. We demonstrate phase mismatch-free nonlinear generation using intrapulse four-wave mixing, where we observed a forward-to-backward nonlinear emission ratio close to unity. The removal of phase matching in nonlinear optical metamaterials may lead to applications such as multidirectional frequency conversion and entangled photon generation.

The ability to pattern optical circuits on-chip, along with coupling in single and entangled photon sources, provides the basis for an integrated quantum optics platform. Wang et al. demonstrate how they can expand on that platform to fabricate very large quantum optical circuitry. They integrated more than 550 quantum optical components and 16 photon sources on a state-of-the-art single silicon chip, enabling universal generation, control, and analysis of multidimensional entanglement. The results illustrate the power of an integrated quantum optics approach for developing quantum technologies. Science , this issue p. 285 Large-scale integrated quantum optical circuitry is demonstrated on a single silicon chip. The ability to control multidimensional quantum systems is central to the development of advanced quantum technologies. We demonstrate a multidimensional integrated quantum photonic platform able to generate, control, and analyze high-dimensional entanglement. A programmable bipartite entangled system is realized with dimensions up to 15 × 15 on a large-scale silicon photonics quantum circuit. The device integrates more than 550 photonic components on a single chip, including 16 identical photon-pair sources. We verify the high precision, generality, and controllability of our multidimensional technology, and further exploit these abilities to demonstrate previously unexplored quantum applications, such as quantum randomness expansion and self-testing on multidimensional states. Our work provides an experimental platform for the development of multidimensional quantum technologies.

The recent development of ultrafast extreme ultraviolet (XUV) coherent light sources bears great potential for a better understanding of the structure and dynamics of matter. Promising routes are advanced coherent control and nonlinear spectroscopy schemes in the XUV energy range, yielding unprecedented spatial and temporal resolution. However, their implementation has been hampered by the experimental challenge of generating XUV pulse sequences with precisely controlled timing and phase properties. In particular, direct control and manipulation of the phase of individual pulses within an XUV pulse sequence opens exciting possibilities for coherent control and multidimensional spectroscopy, but has not been accomplished. Here, we overcome these constraints in a highly time-stabilized and phase-modulated XUV-pump, XUV-probe experiment, which directly probes the evolution and dephasing of an inner subshell electronic coherence. This approach, avoiding any XUV optics for direct pulse manipulation, opens up extensive applications of advanced nonlinear optics and spectroscopy at XUV wavelengths. Light pulses with controllable parameters are desired for studying the fundamental properties of matter. Here the authors generate and use phase-manipulated and highly time-stable XUV pulse pairs to probe the coherent evolution and dephasing of XUV electronic coherences in helium and argon.

The photoionization of xenon atoms in the 70–100 eV range reveals several fascinating physical phenomena such as a giant resonance induced by the dynamic rearrangement of the electron cloud after photon absorption, an anomalous branching ratio between intermediate Xe + states separated by the spin-orbit interaction and multiple Auger decay processes. These phenomena have been studied in the past, using in particular synchrotron radiation, but without access to real-time dynamics. Here, we study the dynamics of Xe 4 d photoionization on its natural time scale combining attosecond interferometry and coincidence spectroscopy. A time-frequency analysis of the involved transitions allows us to identify two interfering ionization mechanisms: the broad giant dipole resonance with a fast decay time less than 50 as, and a narrow resonance at threshold induced by spin-flip transitions, with much longer decay times of several hundred as. Our results provide insight into the complex electron-spin dynamics of photo-induced phenomena. Here the authors report experiment and theory study of the photoionization of xenon inner shell 4d electron using attosecond pulses. They have identified two ionization paths - one corresponding to broad giant dipole resonance with short decay time and the other involving spin-flip transitions.

Trapping light with noble metal nanostructures overcomes the diffraction limit and can confine light to volumes typically on the order of 30 cubic nanometers. We found that individual atomic features inside the gap of a plasmonic nanoassembly can localize light to volumes well below 1 cubic nanometer (\"picocavities\"), enabling optical experiments on the atomic scale. These atomic features are dynamically formed and disassembled by laser irradiation. Although unstable at room temperature, picocavities can be stabilized at cryogenic temperatures, allowing single atomic cavities to be probed for many minutes. Unlike traditional optomechanical resonators, such extreme optical confinement yields a factor of 10⁶ enhancement of optomechanical coupling between the picocavity field and vibrations of individual molecular bonds. This work sets the basis for developing nanoscale nonlinear quantum optics on the single-molecule level.

Fringe Pattern Analysis for Optical Metrology: Theory, Algorithms, and Applications The main objective of this book is to present the basic theoretical principles and practical applications for the classical interferometric techniques and the most advanced methods in the field of modern fringe pattern analysis applied to optical metrology. A major novelty of this work is the presentation of a unified theoretical framework based on the Fourier description of phase shifting interferometry using the Frequency Transfer Function (FTF) along with the theory of Stochastic Process for the straightforward analysis and synthesis of phase shifting algorithms with desired properties such as spectral response, detuning and signal-to-noise robustness, harmonic rejection, etc.