Helmholtz Institute Jena

The discovery of the enhancement of Raman scattering by molecules adsorbed on nanostructured metal surfaces is a landmark in the history of spectroscopic and analytical techniques. Significant experimental and theoretical effort has been directed toward understanding the surface-enhanced Raman scattering (SERS) effect and demonstrating its potential in various types of ultrasensitive sensing applications in a wide variety of fields. In the 45 years since its discovery, SERS has blossomed into a rich area of research and technology, but additional efforts are still needed before it can be routinely used analytically and in commercial products. In this Review, prominent authors from around the world joined together to summarize the state of the art in understanding and using SERS and to predict what can be expected in the near future in terms of research, applications, and technological development. This Review is dedicated to SERS pioneer and our coauthor, the late Prof. Richard Van Duyne, whom we lost during the preparation of this article.

Loss processes in magnetic nanoparticles are discussed with respect to optimization of the specific loss power (SLP) for application in tumour hyperthermia. Several types of magnetic iron oxide nanoparticles representative for different preparation methods (wet chemical precipitation, grinding, bacterial synthesis, magnetic size fractionation) are the subject of a comparative study of structural and magnetic properties. Since the specific loss power useful for hyperthermia is restricted by serious limitations of the alternating field amplitude and frequency, the effects of the latter are investigated experimentally in detail. The dependence of the SLP on the mean particle size is studied over a broad size range from superparamagnetic up to multidomain particles, and guidelines for achieving large SLP under the constraints valid for the field parameters are derived. Particles with the mean size of 18 nm having a narrow size distribution proved particularly useful. In particular, very high heating power may be delivered by bacterial magnetosomes, the best sample of which showed nearly 1 kW g−1 at 410 kHz and 10 kA m−1. This value may even be exceeded by metallic magnetic particles, as indicated by measurements on cobalt particles.

In the 2015 review paper ‘Petawatt Class Lasers Worldwide’ a comprehensive overview of the current status of high-power facilities of ${>}200~\text{TW}$ was presented. This was largely based on facility specifications, with some description of their uses, for instance in fundamental ultra-high-intensity interactions, secondary source generation, and inertial confinement fusion (ICF). With the 2018 Nobel Prize in Physics being awarded to Professors Donna Strickland and Gerard Mourou for the development of the technique of chirped pulse amplification (CPA), which made these lasers possible, we celebrate by providing a comprehensive update of the current status of ultra-high-power lasers and demonstrate how the technology has developed. We are now in the era of multi-petawatt facilities coming online, with 100 PW lasers being proposed and even under construction. In addition to this there is a pull towards development of industrial and multi-disciplinary applications, which demands much higher repetition rates, delivering high-average powers with higher efficiencies and the use of alternative wavelengths: mid-IR facilities. So apart from a comprehensive update of the current global status, we want to look at what technologies are to be deployed to get to these new regimes, and some of the critical issues facing their development.

Structural and magnetic properties of fine particles of magnetite are investigated with respect to the application for hyperthermia. Magnetic hysteresis losses are measured in dependence on the field amplitude for selected commercial powders and are discussed in terms of grain size and structure of the particles. For ferromagnetic powders as well as for ferrofluids, results of heating experiments within organic gels in a magnetic high frequency field are reported. The heating effect depends strongly on the magnetic properties of the magnetite particles which may vary appreciably for different samples in dependence on the particle size and microstructure. In particular, the transition from ferromagnetic to superparamagnetic behavior causes changes of the loss mechanism, and accordingly, of the heating effect. The maximum attainable heating effect is discussed in terms of common theoretical models. Rise of temperature at the surface of a small heated sample as well as in its immediate neighborhood in the surrounding medium is measured in dependence on time and is compared with solutions of the corresponding heat conductivity problem. Conclusions with respect to clinical applications are given.

The application of surface-enhanced Raman spectroscopy (SERS) in biological and biomedical detection schemes is feasible due to its excellent molecular specificity and high sensitivity as well as the capability of SERS to be performed in complex biological compositions. SERS-based investigation of cells, which are the basic structure and functional unit of organisms, represents the starting point of this review. It is demonstrated that SERS provides a deep understanding of living cells as well as their microenvironment which is needed to assess the development of diseases. The clinical relevance of SERS is proved by its application for the detection of cancer cells and tumour margins under in vivo conditions and examples for theranostic approaches are discussed. This review article provides a comprehensive overview of the recent progress within the last 3 years.

The Beer-Lambert law is unquestionably the most important law in optical spectroscopy and indispensable for the qualitative and quantitative interpretation of spectroscopic data. As such, every spectroscopist should know its limits and potential pitfalls, arising from its application, by heart. It is the goal of this work to review these limits and pitfalls, as well as to provide solutions and explanations to guide the reader. This guidance will allow a deeper understanding of spectral features, which cannot be explained by the Beer-Lambert law, because they arise from electromagnetic effects/the wave nature of light. Those features include band shifts and intensity changes based exclusively upon optical conditions, i. e. the method chosen to record the spectra, the substrate and the form of the sample. As such, the review will be an essential tool towards a full understanding of optical spectra and their quantitative interpretation based not only on oscillator positions, but also on their strengths and damping constants.

We present a semiclassical surface-hopping method which is able to treat arbitrary couplings in molecular systems including all degrees of freedom. A reformulation of the standard surface-hopping scheme in terms of a unitary transformation matrix allows for the description of interactions like spin-orbit coupling or transitions induced by laser fields. The accuracy of our method is demonstrated in two systems. The first one, consisting of two model electronic states, validates the semiclassical approach in the presence of an electric field. In the second one, the dynamics in the IBr molecule in the presence of spin-orbit coupling after laser excitation is investigated. Due to an avoided crossing that originates from spin-orbit coupling, IBr dissociates into two channels: I + Br((2)P3/2) and I + Br*((2)P1/2). In both systems, the obtained results are in very good agreement with those calculated from exact quantum dynamical simulations.

A detailed understanding of the properties of electronic excited states and the reaction mechanisms that molecules undergo after light irradiation is a fundamental ingredient for following light-driven natural processes and for designing novel photonic materials. The aim of this review is to present an overview of the ab initio quantum chemical and time-dependent density functional theory methods that can be used to model spectroscopy and photochemistry in molecular systems. The applicability and limitations of the different methods as well as the main frontiers are discussed. To illustrate the progress achieved by excited-state chemistry in the recent years as well as the main challenges facing computational chemistry, three main applications that reflect the authors' experience are addressed: the UV/Vis spectroscopy of organic molecules, the assignment of absorption and emission bands of organometallic complexes, and finally, the obtainment of non-adiabatic photoinduced pathways mediated by conical intersections. In the latter case, special emphasis is put on the photochemistry of DNA. These applications show that the description of electronically excited states is a rewarding but challenging area of research.

The dynamics of energetic particles in strong electromagnetic fields can be heavily influenced by the energy loss arising from the emission of radiation during acceleration, known as radiation reaction. When interacting with a high-energy electron beam, today's lasers are sufficiently intense to explore the transition between the classical and quantum radiation reaction regimes. We present evidence of radiation reaction in the collision of an ultrarelativistic electron beam generated by laser-wakefield acceleration ( > 500 MeV) with an intense laser pulse (a 0 > 10). We measure an energy loss in the postcollision electron spectrum that is correlated with the detected signal of hard photons ( rays), consistent with a quantum description of radiation reaction. The generated rays have the highest energies yet reported from an all-optical inverse Compton scattering scheme, with critical energy crit > 30 MeV.

Upcoming and planned experiments combining increasingly intense lasers and energetic particle beams will access new regimes of nonlinear, relativistic, quantum effects. This improved experimental capability has driven substantial progress in QED in intense background fields. We review here the advances made during the last decade, with a focus on theory and phenomenology. As ever higher intensities are reached, it becomes necessary to consider processes at higher orders in both the number of scattered particles and the number of loops, and to account for non-perturbative physics (e.g. the Schwinger effect), with extreme intensities requiring resummation of the loop expansion. In addition to increased intensity, experiments will reach higher accuracy, and these improvements are being matched by developments in theory such as in approximation frameworks, the description of finite-size effects, and the range of physical phenomena analysed. Topics on which there has been substantial progress include: radiation reaction, spin and polarisation, nonlinear quantum vacuum effects and connections to other fields including physics beyond the Standard Model.

Self-healing coating based on metallopolymers are prepared and fully characterized. Iron bisterpyridine complexes are incorporated into a polymer network based on methacrylates, resulting in self-healing properties of these materials. Moreover, the influence of the comonomers on the thermal properties is studied in detail.

Substantial energy loss in an electron beam passing through a high-intensity laser provides clear evidence of the radiation reaction, shedding light on how electrons interact with extreme electromagnetic fields.

Electron-positron pair plasmas represent a unique state of matter, whereby there exists an intrinsic and complete symmetry between negatively charged (matter) and positively charged (antimatter) particles. These plasmas play a fundamental role in the dynamics of ultra-massive astrophysical objects and are believed to be associated with the emission of ultra-bright gamma-ray bursts. Despite extensive theoretical modelling, our knowledge of this state of matter is still speculative, owing to the extreme difficulty in recreating neutral matter-antimatter plasmas in the laboratory. Here we show that, by using a compact laser-driven setup, ion-free electron-positron plasmas with unique characteristics can be produced. Their charge neutrality (same amount of matter and antimatter), high-density and small divergence finally open up the possibility of studying electron-positron plasmas in controlled laboratory experiments.

As the Human Genome Project and related efforts identify and determine the DNA sequences of human genes, it is important that highly reliable and efficient mechanisms are found to access individual genetic variation. It is only through a greater understanding of genetic diversity that the true benefit of the Human Genome Project will be realized. One approach, hybridization to high-density arrays of oligonucleotides, is a fast and effective means of accessing this genetic variation. Light-directed chemical synthesis has been used to generate miniaturized, high-density arrays of oligonucleotide probes. Application-specific oligonucleotide probe array designs have been developed for the rapid screening of characterized genes. Dedicated instrumentation and software have been developed for array hybridization, fluorescence detection and data acquisition and analysis. In a specific and challenging application, oligonucleotide probe arrays have been used to screen the reverse transcriptase and protease genes of the highly polymorphic HIV-1 genome to explore genetic diversity and detect mutations conferring resistance to antiviral drugs. Results from this application strongly suggest that oligonucleotide probe arrays will be a powerful tool for rapid investigations in sequence checking, pathogen detection, expression monitoring and DNA molecular recognition.

6-H single-crystal silicon carbide thermo-optic coefficient measurements for ultrahigh temperatures up to 1273

An ultrafast laser delivering 10.4 kW average output power based on a coherent combination of 12 step-index fiber amplifiers is presented. The system emits close-to-transform-limited 254 fs pulses at an 80 MHz repetition rate, and has a high beam quality ( <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML" display="inline"> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:msup> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mi mathvariant="normal">M</mml:mi> </mml:mrow> <mml:mn>2</mml:mn> </mml:msup> </mml:mrow> <mml:mo>≤</mml:mo> <mml:mrow class="MJX-TeXAtom-ORD"> <mml:mn>1.2</mml:mn> </mml:mrow> </mml:math> ) and a low relative intensity noise of 0.56% in the frequency range of 1 Hz to 1 MHz. Automated spatiotemporal alignment allows for hands-off operation.

This work presents a review on the effect of transverse mode instability in high-power fiber laser systems and the corresponding investigations led worldwide over the past decade. This paper includes a description of the experimental observations and the physical origin of this effect, as well as some of the proposed mitigation strategies.

Abstract Machine learning has transformed many fields and has recently found applications in chemistry and materials science. The small datasets commonly found in chemistry sparked the development of sophisticated machine learning approaches that incorporate chemical knowledge for each application and, therefore, require specialized expertise to develop. Here we show that GPT-3, a large language model trained on vast amounts of text extracted from the Internet, can easily be adapted to solve various tasks in chemistry and materials science by fine-tuning it to answer chemical questions in natural language with the correct answer. We compared this approach with dedicated machine learning models for many applications spanning the properties of molecules and materials to the yield of chemical reactions. Surprisingly, our fine-tuned version of GPT-3 can perform comparably to or even outperform conventional machine learning techniques, in particular in the low-data limit. In addition, we can perform inverse design by simply inverting the questions. The ease of use and high performance, especially for small datasets, can impact the fundamental approach to using machine learning in the chemical and material sciences. In addition to a literature search, querying a pre-trained large language model might become a routine way to bootstrap a project by leveraging the collective knowledge encoded in these foundation models, or to provide a baseline for predictive tasks.

We report on the generation of a narrow divergence (${\ensuremath{\theta}}_{\ensuremath{\gamma}}&lt;2.5\text{ }\text{ }\mathrm{mrad}$), multi-MeV (${E}_{\mathrm{max}}\ensuremath{\approx}18\text{ }\text{ }\mathrm{MeV}$) and ultrahigh peak brilliance ($&gt;1.8\ifmmode\times\else\texttimes\fi{}{10}^{20}\text{ }\text{ }\mathrm{photons}\text{ }{\mathrm{s}}^{\ensuremath{-}1}\text{ }{\mathrm{mm}}^{\ensuremath{-}2}\text{ }\text{ }{\mathrm{mrad}}^{\ensuremath{-}2}$ 0.1% BW) $\ensuremath{\gamma}$-ray beam from the scattering of an ultrarelativistic laser-wakefield accelerated electron beam in the field of a relativistically intense laser (dimensionless amplitude ${a}_{0}\ensuremath{\approx}2$). The spectrum of the generated $\ensuremath{\gamma}$-ray beam is measured, with MeV resolution, seamlessly from 6 to 18 MeV, giving clear evidence of the onset of nonlinear relativistic Thomson scattering. To the best of our knowledge, this photon source has the highest peak brilliance in the multi-MeV regime ever reported in the literature.

We present a study of laser-driven ion acceleration with micrometer and submicrometer thick plastic targets. Using laser pulses with high temporal contrast and an intensity of the order of 10^{20} W/cm^{2} we observe proton beams with cutoff energies in excess of 85 MeV and particle numbers of 10^{9} in an energy bin of 1 MeV around this maximum. We show that applying the target normal sheath acceleration mechanism with submicrometer thick targets is a very robust way to achieve such high ion energies and particle fluxes. Our results are backed with 2D particle in cell simulations furthermore predicting cutoff energies above 200 MeV for acceleration based on relativistic transparency. This predicted regime can be probed after a few technically feasible adjustments of the laser and target parameters.