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Tailored Disorder in Photonics: Learning from Nature
Disorder and photonics have long been seen as natural adversaries and designers of optical systems have often driven systems to perfection by minimizing deviations from the ideal design. Especially in the field of photonic crystals and metamaterials but also for optical circuits, disorder has been avoided as a nuisance for many years. However, starting from the very robust structural colors found in nature, scientists learn to analyze and tailor disorder to achieve functionalities beyond what is possible with perfectly ordered or ideal systems alone. This review article covers theoretical and materials aspects of tailored disorder as well as experimental results. Furthermore selected examples are highlighted in greater detail, for which the intentional use of disorder adds additional functionality or provides novel functionality impossible without disorder. © 2021 The Authors. Advanced Optical Materials published by Wiley-VCH GmbH
Infrared and NMR Spectroscopic Fingerprints of the Asymmetric H7 + O3 Complex in Solution
Infrared (IR) absorption in the 1000-3700 cm-1 range and 1 H NMR spectroscopy reveal the existence of an asymmetric protonated water trimer, H7 + O3, in acetonitrile. The core H7 + O3 motif persists in larger protonated water clusters in acetonitrile up to at least 8 water molecules. Quantum mechanics/molecular mechanics (QM/MM) molecular dynamics (MD) simulations reveal irreversible proton transport promoted by propagating the asymmetric H7 + O3 structure in solution. The QM/MM calculations allow for the successful simulation of the measured IR absorption spectra of H7 + O3 in the OH stretch region, which reaffirms the assignment of the H7 + O3 spectra to a hybrid-complex structure: a protonated water dimer strongly hydrogen-bonded to a third water molecule with the proton exchanging between the two possible shared-proton Zundel-like centers. The H7 + O3 structure lends itself to promoting irreversible proton transport in presence of even one additional water molecule. We demonstrate how continuously evolving H7 + O3 structures may support proton transport within larger water solvates.
Kinematics of femtosecond laser-generated plasma expansion: Determination of sub-micron density gradient and collisionality evolution of over-critical laser plasmas
An optical diagnostic based on resonant absorption of laser light in a plasma is introduced and is used for the determination of density scale lengths in the range of 10 nm to >1 μm at the critical surface of an overdense plasma. This diagnostic is also used to extract the plasma collisional frequency, allowing inference of the temporally evolving plasma composition on the tens of femtosecond timescale. This is found to be characterized by two eras: the early time and short scale length expansion (L < 0.1λ), where the interaction is highly collisional and target material dependent, followed by a period of material independent plasma expansion for longer scale lengths (L > 0.1λ); this is consistent with a hydrogen plasma decoupling from the bulk target material. Density gradients and plasma parameters on this scale are of importance to plasma mirror optical performance and comment is made on this theme.
High-order parametric generation of coherent XUV radiation
Extreme ultraviolet (XUV) radiation finds numerous applications in spectroscopy. When the XUV light is generated via high-order harmonic generation (HHG), it may be produced in the form of attosecond pulses, allowing access to unprecedented ultrafast phenomena. However, the HHG efficiency remains limited. Here we present an observation of a new regime of coherent XUV emission which has a potential to provide higher XUV intensity, vital for applications. We explain the process by high-order parametric generation, involving the combined emission of THz and XUV photons, where the phase matching is very robust against ionization. This introduces a way to use higher-energy driving pulses, thus generating more XUV photons.
The patterning toolbox FIB-o-mat: Exploiting the full potential of focused helium ions for nanofabrication
Focused beams of helium ions are a powerful tool for high-fidelity machining with spatial precision below 5 nm. Achieving such a high patterning precision over large areas and for different materials in a reproducible manner, however, is not trivial. Here, we introduce the Python toolbox FIB-o-mat for automated pattern creation and optimization, providing full flexibility to accomplish demanding patterning tasks. FIB-o-mat offers high-level pattern creation, enabling high-fidelity large-area patterning and systematic variations in geometry and raster settings. It also offers low-level beam path creation, providing full control over the beam movement and including sophisticated optimization tools. Three applications showcasing the potential of He ion beam nanofabrication for two-dimensional material systems and devices using FIB-o-mat are presented.
The 1-Megapixel pnCCD detector for the Small Quantum Systems Instrument at the European XFEL: system and operation aspects
The X-ray free-electron lasers that became available during the last decade, like the European XFEL (EuXFEL), place high demands on their instrumentation. Especially at low photon energies below 1 keV, detectors with high sensitivity, and consequently low noise and high quantum efficiency, are required to enable facility users to fully exploit the scientific potential of the photon source. A 1-Megapixel pnCCD detector with a 1024 × 1024 pixel format has been installed and commissioned for imaging applications at the Nano-Sized Quantum System (NQS) station of the Small Quantum System (SQS) instrument at EuXFEL. The instrument is currently operating in the energy range between 0.5 and 3 keV and the NQS station is designed for investigations of the interaction of intense FEL pulses with clusters, nano-particles and small bio-molecules, by combining photo-ion and photo-electron spectroscopy with coherent diffraction imaging techniques. The core of the imaging detector is a pn-type charge coupled device (pnCCD) with a pixel pitch of 75 µm × 75 µm. Depending on the experimental scenario, the pnCCD enables imaging of single photons thanks to its very low electronic noise of 3 e− and high quantum efficiency. Here an overview on the EuXFEL pnCCD detector and the results from the commissioning and first user operation at the SQS experiment in June 2019 are presented. The detailed descriptions of the detector design and capabilities, its implementation at EuXFEL both mechanically and from the controls side as well as important data correction steps aim to provide useful background for users planning and analyzing experiments at EuXFEL and may serve as a benchmark for comparing and planning future endstations at other FELs.
Quantum-Optical Spectrometry in Relativistic Laser-Plasma Interactions Using the High-Harmonic Generation Process: A Proposal
Quantum-optical spectrometry is a recently developed shot-to-shot photon correlation-based method, namely using a quantum spectrometer (QS), that has been used to reveal the quantum optical nature of intense laser–matter interactions and connect the research domains of quantum optics (QO) and strong laser-field physics (SLFP). The method provides the probability of absorbing photons from a driving laser field towards the generation of a strong laser–field interaction product, such as high-order harmonics. In this case, the harmonic spectrum is reflected in the photon number distribution of the infrared (IR) driving field after its interaction with the high harmonic generation medium. The method was implemented in non-relativistic interactions using high harmonics produced by the interaction of strong laser pulses with atoms and semiconductors. Very recently, it was used for the generation of non-classical light states in intense laser–atom interaction, building the basis for studies of quantum electrodynamics in strong laser-field physics and the development of a new class of non-classical light sources for applications in quantum technology. Here, after a brief introduction of the QS method, we will discuss how the QS can be applied in relativistic laser–plasma interactions and become the driving factor for initiating investigations on relativistic quantum electrodynamics.
High-energy few-cycle pulses: post-compression techniques
Contemporary ultrafast science requires reliable sources of high-energy few-cycle light pulses. Currently two methods are capable of generating such pulses: post compression of short laser pulses and optical parametric chirped-pulse amplification (OPCPA). Here we give a comprehensive overview on the post-compression technology based on optical Kerr-effect or ionization, with particular emphasis on energy and power scaling. Relevant types of post compression techniques are discussed including free propagation in bulk materials, multiple-plate continuum generation, multi-pass cells, filaments, photonic-crystal fibers, hollow-core fibers and self-compression techniques. We provide a short theoretical overview of the physics as well as an in-depth description of existing experimental realizations of post compression, especially those that can provide few-cycle pulse duration with mJ-scale pulse energy. The achieved experimental performances of these methods are compared in terms of important figures of merit such as pulse energy, pulse duration, peak power and average power. We give some perspectives at the end to emphasize the expected future trends of this technology. © 2020 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.
Origin of Terahertz Soft-Mode Nonlinearities in Ferroelectric Perovskites
Soft modes are intimately linked to structural instabilities and are key for the understanding of phase transitions. The soft modes in ferroelectrics, for example, map directly the polar order parameter of a crystal lattice. Driving these modes into the nonlinear, frequency-changing regime with intense terahertz (THz) light fields is an efficient way to alter the lattice and, with it, the physical properties. However, recent studies show that the THz electric-field amplitudes triggering a nonlinear soft-mode response are surprisingly low, which raises the question on the microscopic picture behind the origin of this nonlinear response. Here, we use linear and two-dimensional terahertz (2D THz) spectroscopy to unravel the origin of the soft-mode nonlinearities in a strain-engineered epitaxial ferroelectric SrTiO3 thin film. We find that the linear dielectric function of this mode is quantitatively incompatible with pure ionic or pure electronic motions. Instead, 2D THz spectroscopy reveals a pronounced coupling of electronic and ionic-displacement dipoles. Hence, the soft mode is a hybrid mode of lattice (ionic) motions and electronic interband transitions. We confirm this conclusion with model calculations based on a simplified pseudopotential concept of the electronic band structure. It reveals that the entire THz nonlinearity is caused by the off-resonant nonlinear response of the electronic interband transitions of the lattice-electronic hybrid mode. With this work, we provide fundamental insights into the microscopic processes that govern the softness that any material assumes near a ferroic phase transition. This knowledge will allow us to gain an efficient all-optical control over the associated large nonlinear effects.
8 fs laser pulses from a compact gas-filled multi-pass cell
Compression of 42 fs, 0.29 mJ pulses from a Ti:Sapphire amplifier down to 8 fs (approximately 3 optical cycles) is demonstrated by means of spectral broadening in a compact multi-pass cell filled with argon. The efficiency of the nonlinear pulse compression is limited to 45 % mostly by losses in the mirrors of the cell. The experimental results are supported by 3-dimensional numerical simulations of the nonlinear pulse propagation in the cell that allow us to study spatio-spectral properties of the pulses after spectral broadening.