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Waveguide-Integrated Broadband Spectrometer Based on Tailored Disorder

2020, Hartmann, Wladick, Varytis, Paris, Gehring, Helge, Walter, Nicolai, Beutel, Fabian, Busch, Kurt, Pernice, Wolfram

Compact, on-chip spectrometers exploiting tailored disorder for broadband light scattering enable high-resolution signal analysis while maintaining a small device footprint. Due to multiple scattering events of light in the disordered medium, the effective path length of the device is significantly enhanced. Here, on-chip spectrometers are realized for visible and near-infrared wavelengths by combining an efficient broadband fiber-to-chip coupling approach with a scattering area in a broadband transparent silicon nitride waveguiding structure. Air holes etched into a structured silicon nitride slab terminated with multiple waveguides enable multipath light scattering in a diffusive regime. Spectral-to-spatial mapping is performed by determining the transmission matrix at the waveguide outputs, which is then used to reconstruct the probe signals. Direct comparison with theoretical analyses shows that such devices can be used for high-resolution spectroscopy from the visible up to the telecom wavelength regime. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

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High-energy few-cycle pulses: post-compression techniques

2021, Nagy, Tamas, Simon, Peter, Veisz, Laszlo

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.

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Nanostructured In3SbTe2 antennas enable switching from sharp dielectric to broad plasmonic resonances

2022, Heßler, Andreas, Wahl, Sophia, Kristensen, Philip Trøst, Wuttig, Matthias, Busch, Kurt, Taubner, Thomas

Phase-change materials (PCMs) allow for non-volatile resonance tuning of nanophotonic components. Upon switching, they offer a large dielectric contrast between their amorphous and crystalline phases. The recently introduced “plasmonic PCM” In3SbTe2 (IST) additionally features in its crystalline phase a sign change of its permittivity over a broad infrared spectral range. While optical resonance switching in unpatterned IST thin films has been investigated before, nanostructured IST antennas have not been studied, yet. Here, we present numerical and experimental investigations of nanostructured IST rod and disk antennas. By crystallizing the IST with microsecond laser pulses, we switched individual antennas from narrow dielectric to broad plasmonic resonances. For the rod antennas, we demonstrated a resonance shift of up to 1.2 µm (twice the resonance width), allowing on/off switching of plasmonic resonances with a contrast ratio of 2.7. With the disk antennas, we realized an increase of the resonance width by more than 800% from 0.24 µm to 1.98 µm while keeping the resonance wavelength constant. Further, we demonstrated intermediate switching states by tuning the crystallization depth within the resonators. Our work empowers future design concepts for nanophotonic applications like active spectral filters, tunable absorbers, and switchable flat optics.

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Robust transverse structures in rescattered photoelectron wavepackets and their consequences

2020, Bredtmann, T., Patchkovskii, S.

Initial-state symmetry has been under-appreciated in strong-field spectroscopies, where laser fields dominate the dynamics. We demonstrate numerically that the transverse photoelectron phase structure, arising from the initial-state symmetry, is robust in strong-field rescattering, and has pronounced effects on strong-field photoelectron spectra. Interpretation of rescattering experiments need to take these symmetry effects into account. In turn, robust transverse photoelectron phase structures may enable attosecond sub-Ångström super-resolution imaging with structured electron beams.

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Short-Range Cooperative Slow-down of Water Solvation Dynamics Around SO42--Mg2+ Ion Pairs

2022, Kundu, Achintya, Mamatkulov, Shavkat I., Brünig, Florian N., Bonthuis, Douwe Jan, Netz, Roland R., Elsaesser, Thomas, Fingerhut, Benjamin P.

The presence of ions affects the structure and dynamics of water on a multitude of length and time scales. In this context, pairs of Mg2+ and SO42- ions in water constitute a prototypical system for which conflicting pictures of hydration geometries and dynamics have been reported. Key issues are the molecular pair and solvation shell geometries, the spatial range of electric interactions, and their impact on solvation dynamics. Here, we introduce asymmetric SO42- stretching vibrations as new and most specific local probes of solvation dynamics that allow to access ion hydration dynamics at the dilute concentration (0.2 M) of a native electrolyte environment. Highly sensitive heterodyne 2D-IR spectroscopy in the fingerprint region of the SO42- ions around 1100 cm-1 reveals a specific slow-down of solvation dynamics for hydrated MgSO4 and for Na2SO4 in the presence of Mg2+ ions, which manifests as a retardation of spectral diffusion compared to aqueous Na2SO4 solutions in the absence of Mg2+ ions. Extensive molecular dynamics and density functional theory QM/MM simulations provide a microscopic view of the observed ultrafast dephasing and hydration dynamics. They suggest a molecular picture where the slow-down of hydration dynamics arises from the structural peculiarities of solvent-shared SO42--Mg2+ ion pairs.

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Needle beams: a review

2020, Grunwald R., Bock M.

Needle beams are highly attractive for applications which take advantage from a spatial and temporal localization of photons. High intensities, high resolution and extended depth of focus lead to fundamental advances in the optical system performance. Ultrashort, fringe-free, self-reconstructing nondiffracting pulses with undistorted temporal transfer are obtained by generating truncated Bessel beams under self-apodization conditions. Nondiffracting Talbot self-imaging of needle beam arrays enables to transfer near field information to the Fraunhofer zone. With addressable arrays of needle beams, reconfigurable time-wavefront sensors are built up. Moreover, spatial light modulators and flexible axicons are used to realize structured, highly localized wavepackets, accelerating beams and nondiffracting images. © 2020, © 2020 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.

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A general approach for all-visible-light switching of diarylethenes through triplet sensitization using semiconducting nanocrystals

2022, Hou, Lili, Larsson, Wera, Hecht, Stefan, Andréasson, Joakim, Albinsson, Bo

Coupling semiconducting nanocrystals (NCs) with organic molecules provides an efficient route to generate and transfer triplet excitons. These excitons can be used to power photochemical transformations such as photoisomerization reactions using low energy radiation. Thus, it is desirable to develop a general approach that can efficiently be used to control photoswitches using all-visible-light aiming at future applications in life- and materials sciences. Here, we demonstrate a simple ‘cocktail’ strategy that can achieve all-visible-light switchable diarylethenes (DAEs) through triplet energy transfer from the hybrid of CdS NCs and phenanthrene-3-carboxylic acid, with high photoisomerization efficiency and improved fatigue resistance. The size-tunable excitation energies of CdS NCs make it possible to precisely match the clear spectral window of the relevant DAE photoswitch. We demonstrate reversible all-visible-light photoisomerization of a series of DAE derivatives both in the liquid and solid state, even in the presence of oxygen. Our general strategy is promising for fabrication of all-visible-light activated optoelectronic devices as well as memories, and should in principle be adaptable to photopharmacology.

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Tailored Disorder in Photonics: Learning from Nature

2021, Rothammer, Maximilian, Zollfrank, Cordt, Busch, Kurt, Freymann, Georg von

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

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Infrared emission bands and thermal effects for 440-nm-emitting GaN-based laser diodes

2020, Mao F., Hong J., Wang H., Chen Y., Jing C., Yang P., Tomm J.W., Chu J., Yue F.

Broad emission bands due to defects in (In,Ga,Al)N laser diodes operating at 440 nm are investigated using continuous-wave and pulsed currents. In addition to known yellow-green and short-wave infrared bands, defect emissions were observed even in the medium-wave infrared range. A separation from thermal radiation is possible. When using pulsed currents, a super-linearly increasing emission occurs at ∼1150 nm, which could be attributed to amplified spontaneous emission mainly due to the electroluminescence of deep defects in the optically active region. These results may be useful in interpreting the output power bottleneck of GaN-based lasers compared to mature GaAs-based lasers. © 2020 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/). https://doi.org/10.1063/1.5143802

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Delayed relaxation of highly excited naphthalene cations

2020, Reitsma, G., Hummert, J., Dura, J., Loriot, V., Vrakking, M.J.J., Lépine, F., Kornilov, O.

The efficiency of energy transfer in ultrafast electronic relaxation of molecules depends strongly on the complex interplay between electronic and nuclear motion. In this study we use wavelength-selected XUV pulses to induce relaxation dynamics of highly excited cationic states of naphthalene. Surprisingly, the observed relaxation lifetimes increase with the cationic excitation energy. We propose that this is a manifestation of a quantum mechanical population trapping that leads to delayed relaxation of molecules in the regions with a high density of excited states. © 2019 Published under licence by IOP Publishing Ltd.