Terahertz-slicing - an all-optical synchronization for 4th generation light sources.

A conceptually new approach to synchronizing accelerator-based light sources and external laser systems is presented. The concept is based on utilizing a sufficiently intense accelerator-based single-cycle terahertz pulse to slice a thereby intrinsically synchronized femtosecond-level part of a longer picosecond laser pulse in an electro-optic crystal. A precise synchronization of the order of 10 fs is demonstrated, allowing for real-time lock-in amplifier signal demodulation. We demonstrate successful operation of the concept with three benchmark experiments using a 4th generation accelerator-based terahertz light source, i.e. (i) far-field terahertz time-domain spectroscopy, (ii) terahertz high harmonic generation spectroscopy, and (iii) terahertz scattering-type scanning near-field optical microscopy.

Fiber-dispersive Raman spectrometer with single-photon sensitivity.

The two major challenges in Raman spectroscopy are the low intensity of spontaneous Raman scattering and often accompanying luminescence. We overcome these two issues with a novel fiber-dispersive Raman spectrometer utilizing pulsed excitation and a superconducting nanowire single-photon detector (SNSPD). By exploiting chromatic dispersion in the fiber material, we stretched propagation times of Raman photons and performed correlated measurements in the time domain, where the two emission processes, Raman scattering and luminescence, can be effectively separated. The spectrometer greatly benefits from SNSPD metrics, i.e. broad spectral sensitivity (from UV to near-IR wavelength range) on a single-photon level and high timing resolution (small timing jitter), which outperform those of competing avalanche single-photon detectors. The spectral resolution achievable with a fiber-dispersive spectrometer for the optimized components is estimated to be as good as 3 - 10 cm-1 over the Stokes shifted range up to 4400 cm-1 with an excitation wavelength of 785 nm and below 5 cm-1 covering the same range with an excitation wavelength of 532 nm.

Volt-per-Ångstrom terahertz fields from X-ray free-electron lasers.

The electron linear accelerators driving modern X-ray free-electron lasers can emit intense, tunable, quasi-monochromatic terahertz (THz) transients with peak electric fields of V Å-1 and peak magnetic fields in excess of 10 T when a purpose-built, compact, superconducting THz undulator is implemented. New research avenues such as X-ray movies of THz-driven mode-selective chemistry come into reach by making dual use of the ultra-short GeV electron bunches, possible by a rather minor extension of the infrastructure.

Pulse- and field-resolved THz-diagnostics at 4 t h generation lightsources.

Multi-color pump-probe techniques utilizing modern accelerator-based 4th generation light sources such as X-ray free electron lasers or superradiant THz facilities have become important science drivers over the past 10 years. In this type of experiments the precise knowledge of the properties of the involved accelerator-based light pulses crucially determines the achievable sensitivity and temporal resolution. In this work we demonstrate and discuss the powerful role pulse- and field-resolved- detection of superradiant THz pulses can play for improving the precision of THz pump - femtosecond laser probe experiments at superradiant THz facilities in particular and at 4th generation light sources in general. The developed diagnostic scheme provides real-time information on the properties of individual pulses from multiple accelerator based THz sources and opens a robust way for sub femtosecond timing. Correlations between amplitude and phase of the pulses emitted from different superradiant THz sources furthermore provide insides into the properties of the driving electron bunches and is of general interest for the ultra-fast diagnostics at 4th generation light sources.

On-chip THz spectrometer for bunch compression fingerprinting at fourth-generation light sources.

The layout of an integrated millimetre-scale on-chip THz spectrometer is presented and its peformance demonstrated. The device is based on eight Schottky-diode detectors which are combined with narrowband THz antennas, thereby enabling the simultaneous detection of eight frequencies in the THz range on one chip. The size of the active detector area matches the focal spot size of superradiant THz radiation utilized in bunch compression monitors of modern linear electron accelerators. The 3 dB bandwidth of the on-chip Schottky-diode detectors is less than 10% of the center frequency and allows pulse-resolved detection at up to 5 GHz repetition rates. The performance of a first prototype device is demonstrated at a repetition rate of 100 kHz at the quasi-cw SRF linear accelerator ELBE operated with electron bunch charges between a few pC and 100 pC.

Towards femtosecond-level intrinsic laser synchronization at fourth generation light sources.

In this Letter, the proof of principle for a scheme providing intrinsic femtosecond-level synchronization between an external laser system and fourth generation light sources is presented. The scheme is applicable at any accelerator-based light source that is based on the generation of coherent radiation from ultrashort electron bunches such as superradiant terahertz (THz) facilities or X-FELs. It makes use of a superradiant THz pulse generated by the accelerator as an intrinsically synchronized gate signal for electro-optical slicing. We demonstrate that the scheme enables a reduction of the timing instability by more than 2 orders of magnitude. This demonstration experiment thereby proves that intrinsically synchronized time-resolved experiments utilizing laser and accelerator-based radiation pulses on few tens of femtosecond (fs) to few fs timescales are feasible.

Magnetic Excitations and Continuum of a Possibly Field-Induced Quantum Spin Liquid in α-RuCl_{3}.

We report on terahertz spectroscopy of quantum spin dynamics in α-RuCl_{3}, a system proximate to the Kitaev honeycomb model, as a function of temperature and magnetic field. We follow the evolution of an extended magnetic continuum below the structural phase transition at T_{s2}=62 K. With the onset of a long-range magnetic order at T_{N}=6.5 K, spectral weight is transferred to a well-defined magnetic excitation at ℏω_{1}=2.48 meV, which is accompanied by a higher-energy band at ℏω_{2}=6.48 meV. Both excitations soften in a magnetic field, signaling a quantum phase transition close to B_{c}=7 T, where a broad continuum dominates the dynamical response. Above B_{c}, the long-range order is suppressed, and on top of the continuum, emergent magnetic excitations evolve. These excitations follow clear selection rules and exhibit distinct field dependencies, characterizing the dynamical properties of a possibly field-induced quantum spin liquid.

Probing ultra-fast processes with high dynamic range at 4th-generation light sources: Arrival time and intensity binning at unprecedented repetition rates.

Understanding dynamics on ultrafast timescales enables unique and new insights into important processes in the materials and life sciences. In this respect, the fundamental pump-probe approach based on ultra-short photon pulses aims at the creation of stroboscopic movies. Performing such experiments at one of the many recently established accelerator-based 4th-generation light sources such as free-electron lasers or superradiant THz sources allows an enormous widening of the accessible parameter space for the excitation and/or probing light pulses. Compared to table-top devices, critical issues of this type of experiment are fluctuations of the timing between the accelerator and external laser systems and intensity instabilities of the accelerator-based photon sources. Existing solutions have so far been only demonstrated at low repetition rates and/or achieved a limited dynamic range in comparison to table-top experiments, while the 4th generation of accelerator-based light sources is based on superconducting radio-frequency technology, which enables operation at MHz or even GHz repetition rates. In this article, we present the successful demonstration of ultra-fast accelerator-laser pump-probe experiments performed at an unprecedentedly high repetition rate in the few-hundred-kHz regime and with a currently achievable optimal time resolution of 13 fs (rms). Our scheme, based on the pulse-resolved detection of multiple beam parameters relevant for the experiment, allows us to achieve an excellent sensitivity in real-world ultra-fast experiments, as demonstrated for the example of THz-field-driven coherent spin precession.

High-Field High-Repetition-Rate Sources for the Coherent THz Control of Matter.

Ultrashort flashes of THz light with low photon energies of a few meV, but strong electric or magnetic field transients have recently been employed to prepare various fascinating nonequilibrium states in matter. Here we present a new class of sources based on superradiant enhancement of radiation from relativistic electron bunches in a compact electron accelerator that we believe will revolutionize experiments in this field. Our prototype source generates high-field THz pulses at unprecedented quasi-continuous-wave repetition rates up to the MHz regime. We demonstrate parameters that exceed state-of-the-art laser-based sources by more than 2 orders of magnitude. The peak fields and the repetition rates are highly scalable and once fully operational this type of sources will routinely provide 1 MV/cm electric fields and 0.3 T magnetic fields at repetition rates of few 100 kHz. We benchmark the unique properties by performing a resonant coherent THz control experiment with few 10 fs resolution.

Single-pulse picking at kHz repetition rates using a Ge plasma switch at the free-electron laser FELBE.

We demonstrate a system for picking of mid-infrared and terahertz (THz) radiation pulses from the free-electron laser (FEL) FELBE operating at a repetition rate of 13 MHz. Single pulses are reflected by a dense electron-hole plasma in a Ge slab that is photoexcited by amplified near-infrared (NIR) laser systems operating at repetition rates of 1 kHz and 100 kHz, respectively. The peak intensity of picked pulses is up to 400 times larger than the peak intensity of residual pulses. The required NIR fluence for picking pulses at wavelengths in the range from 5 µm to 30 µm is discussed. In addition, we show that the reflectivity of the plasma decays on a time scale from 100 ps to 1 ns dependent on the wavelengths of the FEL and the NIR laser. The plasma switch enables experiments with the FEL that require high peak power but lower average power. Furthermore, the system is well suited to investigate processes with decay times in the µs to ms regime, i.e., much longer than the 77 ns long pulse repetition period of FELBE.

Optical nanoscopy of transient states in condensed matter.

Recently, the fundamental and nanoscale understanding of complex phenomena in materials research and the life sciences, witnessed considerable progress. However, elucidating the underlying mechanisms, governed by entangled degrees of freedom such as lattice, spin, orbit, and charge for solids or conformation, electric potentials, and ligands for proteins, has remained challenging. Techniques that allow for distinguishing between different contributions to these processes are hence urgently required. In this paper we demonstrate the application of scattering-type scanning near-field optical microscopy (s-SNOM) as a novel type of nano-probe for tracking transient states of matter. We introduce a sideband-demodulation technique that allows for probing exclusively the stimuli-induced change of near-field optical properties. We exemplify this development by inspecting the decay of an electron-hole plasma generated in SiGe thin films through near-infrared laser pulses. Our approach can universally be applied to optically track ultrafast/-slow processes over the whole spectral range from UV to THz frequencies.

Single-shot pulse duration monitor for extreme ultraviolet and X-ray free-electron lasers.

The resolution of ultrafast studies performed at extreme ultraviolet and X-ray free-electron lasers is still limited by shot-to-shot variations of the temporal pulse characteristics. Here we show a versatile single-shot temporal diagnostic tool that allows the determination of the extreme ultraviolet pulse duration and the relative arrival time with respect to an external pump-probe laser pulse. This method is based on time-resolved optical probing of the transient reflectivity change due to linear absorption of the extreme ultraviolet pulse within a solid material. In this work, we present measurements performed at the FLASH free-electron laser. We determine the pulse duration at two distinct wavelengths, yielding (184±14) fs at 41.5 nm and (21±19) fs at 5.5 nm. Furthermore, we demonstrate the feasibility to operate the tool as an online diagnostic by using a 20-nm-thin Si3N4 membrane as target. Our results are supported by detailed numerical and analytical investigations.

Optical excitation of Josephson plasma solitons in a cuprate superconductor.

Josephson plasma waves are linear electromagnetic modes that propagate along the planes of cuprate superconductors, sustained by interlayer tunnelling supercurrents. For strong electromagnetic fields, as the supercurrents approach the critical value, the electrodynamics become highly nonlinear. Josephson plasma solitons (JPSs) are breather excitations predicted in this regime, bound vortex-antivortex pairs that propagate coherently without dispersion. We experimentally demonstrate the excitation of a JPS in La1.84Sr0.16CuO4, using intense narrowband radiation from an infrared free-electron laser tuned to the 2-THz Josephson plasma resonance. The JPS becomes observable as it causes a transparency window in the opaque spectral region immediately below the plasma resonance. Optical control of magnetic-flux-carrying solitons may lead to new applications in terahertz-frequency plasmonics, in information storage and transport and in the manipulation of high-Tc superconductivity.

Evidence for chirped Auger-electron emission.

Auger decay carries valuable information about the electronic structure and dynamics of atoms, molecules, and solids. Here we furnish evidence that under certain conditions Auger electrons are subject to an energetic chirp. The effect is disclosed in time-resolved streaking experiments on the Xe NOO and Kr MNN Auger decay using extreme-ultraviolet pulses from the free-electron laser in Hamburg as well as from a high-order harmonic laser source. The origin of this effect is found to be an exchange of energy between the Auger electron and an earlier emitted correlated photoelectron. The observed time-dependent spectral modulations are understood within an analytical model and confirmed by extensive computer simulations.

Photoinduced melting of antiferromagnetic order in La(0.5)Sr(1.5)MnO4 measured using ultrafast resonant soft x-ray diffraction.

We used ultrafast resonant soft x-ray diffraction to probe the picosecond dynamics of spin and orbital order in La(0.5)Sr(1.5)MnO(4) after photoexcitation with a femtosecond pulse of 1.5 eV radiation. Complete melting of antiferromagnetic spin order is evidenced by the disappearance of a (1/4,1/4,1/2) diffraction peak. On the other hand, the (1/4,1/4,0) diffraction peak, reflecting orbital order, is only partially reduced. We interpret the results as evidence of destabilization in the short-range exchange pattern with no significant relaxation of the long-range Jahn-Teller distortions. Cluster calculations are used to analyze different possible magnetically ordered states in the long-lived metastable phase. Nonthermal coupling between light and magnetism emerges as a primary aspect of photoinduced phase transitions in manganites.

Positive effect of HPA lanolin versus expressed breastmilk on painful and damaged nipples during lactation.

Painful and/or damaged nipples associated with breastfeeding are common and represent a challenge for both the persons experiencing nipple pain and/or trauma and for those providing treatment. However, evidence-based data has been insufficient to demonstrably minimize these common reasons for failure to initiate or continue successful breastfeeding. The aim of this study was to evaluate the efficacy of specific-grade highly purified anhydrous (HPA) lanolin versus expressed breastmilk (EBM) for the treatment of painful and damaged nipples associated with breastfeeding in a prospective controlled clinical trial evaluating 84 lactating mothers. Nipple trauma and healing rates were rated by the Nipple Trauma Score. Nipple pain intensity was assessed on a visual analog scale. Outcome parameters were in favor of the HPA lanolin group, reaching statistical significance for healing rates, nipple trauma and nipple pain. In our study, we found HPA lanolin more effective than EBM, inducing faster healing of nipple trauma (absolute risk reduction of 0.43) and reducing nipple pain (absolute risk reduction of 0.61 on day 3). We concluded that HPA lanolin, combined with breastfeeding education, was more effective than EBM, combined with breastfeeding education, in reducing nipple pain and promoting healing of nipple trauma.

Structure of si(111)-in nanowires determined from the midinfrared optical response.

The anisotropic optical response of Si(111)-(4x1)/(8x2)-In in the midinfrared, where ab initio studies predict significant changes in the band structure between competing models of this important quasi-1D system, has been measured using infrared spectroscopic ellipsometry (IRSE) and reflection anisotropy spectroscopy (RAS). Both IRSE and RAS of the (8x2) phase show that the anisotropic Drude tail of the (4x1) phase is replaced by two peaks at 0.50 and 0.72 eV, which appear in ab initio optical response calculations for the hexagon model of the (8x2) structure, but not the trimer model.

Few-photon multiple ionization of N2 by extreme ultraviolet free-electron laser radiation.

Few-photon multiple ionization of N2 was studied differentially in a reaction microscope using 44 eV, approximately 25 fs, intense ( approximately 10(13) W/cm(2)) photon pulses from FLASH. Sequential ionization is observed to dominate. For various intermediate charge states N(2)(n+0 we find a considerable excess of photons absorbed compared to the minimum number that would energetically be required. Photoionization of aligned N(2)(n+) ions, produced by photon absorption in sequential steps, is explored and few-photon absorption pathways are traced by inspecting kinetic energy releases and fragment-ion angular distributions.

Recoil-ion momentum distributions for two-photon double ionization of He and Ne by 44 eV free-electron laser radiation.

Recoil-ion momentum distributions for two-photon double ionization of He and Ne (variant Planck's over omega=44 eV) have been recorded with a reaction microscope at FLASH (the free-electron laser at Hamburg) at an intensity of approximately 1 x 10(14) W/cm2 exploring the dynamics of the two fundamental two-photon-two-electron reaction pathways, namely, sequential and direct (or nonsequential) absorption of the photons. We find strong differences in the recoil-ion momentum patterns for the two mechanisms pointing to the significantly different two-electron emission dynamics and thus provide serious constraints for theoretical models.

Time-resolved synchrotron XPS monitoring of irradiation-induced nitrobenzene reduction for chemical lithography.

The irradiation-induced reduction of electrochemically grafted nitrobenzene films on Si(111) was monitored by high-resolution photoelectron spectroscopy. The experiments were performed using synchrotron soft X-ray irradiation at the BESSY II synchrotron facility. The evolution of different chemical species was monitored as a function of time. Careful fitting of the Si2p, C1s, N1s, and O1s core level spectra allowed us to follow this process in detail and to determine the constants of growth and decay of the specific components. The chemical changes were caused by the X-ray irradiation-induced secondary electron current through the aryl layer. A minor fraction (approximately 25%) of the initial nitro groups was split off and desorbed. The bulk of the NO2 groups was reduced to species in an amino-like chemical environment. A desorption of carbon fragments was not observed, and benzene ring specific shakeup satellites indicated that the aromatic ring structure remained intact. Irradiation-induced line-shape changes suggest a polymerization via -NH- bridges, which were formed after the irradiation-induced N-O bond splitting. A significant part of the released oxygen appeared to contribute to an oxidation of the silicon substrate at the Si(111)/benzene interface. The irradiation-induced aryl layer modification can be exploited for chemical lithography (i.e., a lateral structuring of functionalized silicon surfaces).