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- ItemShort-Range Cooperative Slow-down of Water Solvation Dynamics Around SO42--Mg2+ Ion Pairs(Washington, DC : American Chemical Society, 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.
- ItemTailored Disorder in Photonics: Learning from Nature(Weinheim : Wiley-VCH, 2021) Rothammer, Maximilian; Zollfrank, Cordt; Busch, Kurt; Freymann, Georg vonDisorder 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
- ItemHigh-energy few-cycle pulses: post-compression techniques(Abingdon : Taylor & Francis Group, 2021) Nagy, Tamas; Simon, Peter; Veisz, LaszloContemporary 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.
- ItemNanostructured In3SbTe2 antennas enable switching from sharp dielectric to broad plasmonic resonances(Berlin : de Gruyter, 2022) Heßler, Andreas; Wahl, Sophia; Kristensen, Philip Trøst; Wuttig, Matthias; Busch, Kurt; Taubner, ThomasPhase-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.
- ItemA general approach for all-visible-light switching of diarylethenes through triplet sensitization using semiconducting nanocrystals(London [u.a.] : RSC, 2022) Hou, Lili; Larsson, Wera; Hecht, Stefan; Andréasson, Joakim; Albinsson, BoCoupling 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.
- ItemHigh power, high repetition rate laser-based sources for attosecond science(Bristol : IOP Publishing, 2022) Furch, F.J.; Witting, T.; Osolodkov, M.; Schell, F.; Schulz, C.P.; Vrakking, M.J.Within the last two decades attosecond science has been established as a novel research field providing insights into the ultrafast electron dynamics that follows a photoexcitation or photoionization process. Enabled by technological advances in ultrafast laser amplifiers, attosecond science has been in turn, a powerful engine driving the development of novel sources of intense ultrafast laser pulses. This article focuses on the development of high repetition rate laser-based sources delivering high energy pulses with a duration of only a few optical cycles, for applications in attosecond science. In particular, a high power, high repetition rate optical parametric chirped pulse amplification system is described, which was developed to drive an attosecond pump-probe beamline targeting photoionization experiments with electron-ion coincidence detection at high acquisition rates.
- ItemOrigin of Terahertz Soft-Mode Nonlinearities in Ferroelectric Perovskites(College Park, Md. : APS, 2021) Pal, Shovon; Strkalj, Nives; Yang, Chia-Jung; Weber, Mads C.; Trassin, Morgan; Woerner, Michael; Fiebig, ManfredSoft 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.
- ItemGeneral Time-Dependent Configuration-Interaction Singles II: The Atomic Case(Woodbury, NY : Inst., 2022-10-10) Carlström, Stefanos; Bertolino, Mattias; Dahlström, Jan Marcus; Patchkovskii, SergueiWe present a specialization of the grid-based implementation of the time-dependent configuration-interaction singles described in the preceding paper [S. Carlström et al., preceding paper, Phys. Rev. A 106, 043104 (2022)]. to the case of spherical symmetry. We describe the intricate time propagator in detail and conclude with a few example calculations. Among these, of note are high-resolution photoelectron spectra in the vicinity of the Fano resonances in photoionization of neon and spin-polarized photoelectrons from xenon, in agreement with recent experiments.
- ItemGeneral Time-Dependent Configuration-Interaction Singles I: The Molecular Case(Woodbury, NY : Inst., 2022-10-10) Carlström, Stefanos; Spanner, Michael; Patchkovskii, SergueiWe present a grid-based implementation of the time-dependent configuration-interaction singles method suitable for computing the strong-field ionization of small gas-phase molecules. After outlining the general equations of motion used in our treatment of this method, we present example calculations of strong-field ionization of He, LiH, H2O, and C2H4 that demonstrate the utility of our implementation. The following paper [S. Carlström et al., following paper, Phys. Rev. A 106, 042806 (2022)] specializes to the case of spherical symmetry, which is applied to various atoms.
- ItemKinematics of femtosecond laser-generated plasma expansion: Determination of sub-micron density gradient and collisionality evolution of over-critical laser plasmas([S.l.] : American Institute of Physics, 2021) Scott, G.G.; Indorf, G.F.H.; Ennen, M.A.; Forestier-Colleoni, P.; Hawkes, S.J.; Scaife, L.; Sedov, M.; Symes, D.R.; Thornton, C.; Beg, F.; Ma, T.; McKenna, P.; Andreev, A.A.; Teubner, U.; Neely, D.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.