Magnetic Excitations and Continuum of a Field-Induced Quantum Spin Liquid in α\alpha-RuCl3_3

We report on terahertz spectroscopy of quantum spin dynamics in $\alpha$-RuCl$_3$, a system proximate to the Kitaev honeycomb model, as a function of temperature and magnetic field. An extended magnetic continuum develops 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 $\hbar \omega_1 = 2.48$meV, which is accompanied by a higher-energy band at $\hbar \omega_2 = 6.48$meV. Both excitations soften in magnetic field, signaling a quantum phase transition at $B_c=7$T where we find a broad continuum dominating the dynamical response. Above $B_c$, the long-range order is suppressed, and on top of the continuum, various emergent magnetic excitations evolve. These excitations follow clear selection rules and exhibit distinct field dependencies, characterizing the dynamical properties of the field-induced quantum spin liquid

Inhomogeneity of donor doping in SrTiO3 substrates studied by fluorescence-lifetime imaging microscopy

Fluorescence-lifetime imaging microscopy (FLIM) was applied to investigate the donor distribution in SrTiO3 single crystals. On the surfaces of Nb- and La-doped SrTiO3, structures with different fluorescence intensities and lifetimes were found that could be related to different concentrations of Ti3+. Furthermore, the inhomogeneous distribution of donors caused a non-uniform conductivity of the surface, which complicates the production of potential electronic devices by the deposition of oxide thin films on top of doped single crystals. Hence, we propose FLIM as a convenient technique (length scale: 1 $\mu$m) for characterizing the quality of doped oxide surfaces, which could help to identify appropriate substrate materials

Magnetic field dependence of antiferromagnetic resonance in NiO

We report on measurements of magnetic field and temperature dependence of antiferromagnetic resonances in the prototypical antiferromagnet NiO. The frequencies of the magnetic resonances in the vicinity of 1 THz have been determined in the time-domain via time-resolved Faraday measurements after selective excitation by narrow-band superradiant terahertz (THz) pulses at temperatures down to 3 K and in magnetic fields up to 10 T. The measurements reveal two antiferromagnetic resonance modes, which can be distinguished by their characteristic magnetic field dependencies. The nature of the two modes is discussed by comparison to an eight-sublattice antiferromagnetic model, which includes superexchange between the next-nearest-neighbor Ni spins, magnetic dipolar interactions, cubic magneto-crystalline anisotropy, and Zeeman interaction with the external magnetic field. Our study indicates that a two-sublattice model is insufficient for the description of spin dynamics in NiO, while the magnetic-dipolar interactions and magneto-crystalline anisotropy play important roles

Polarisation Sensitive Single Molecule Fluorescence Detection with Linear Polarised Excitation Light and Modulated Polarisation Direction Applied to Multichromophoric Entities

Recently, investigations of the fluorescence properties of a multichromophoric dendritic entity at the single molecule level have revealed multiple fluorescence levels, collective off-states, variations of the polarisation, large shifts in the spectral position and changes in the fluorescence decay time. In order to further elucidate the multiple processes taking place in this entity, measurements were done in which the polarisation direction of the linear polarised excitation light was modulated. The detection was sensitive for the s- and p-components of the emitted light. The patterns of modulation and relative intensity in the acquired traces reflect the energy transfer processes occurring in this multichromophoric molecule. In-phase modulation and no modulation are the typical modulation patterns that were observed. Simulations involving several models for energy transfer between the chromophores have been carried out taking into account identical conditions as for the performed measurements. The comparison of the modulation patterns and polarisation histograms to the measured data rules out certain models and refines the photophysical model for the multichromophoric entity

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

Intramolecular evolution from a locally excited state to an excimer-like state in a multichromophoric dendrimer evidenced by a femtosecond fluorescence upconversion study

A time-resolved fluorescence upconversion study on a polyphenylene dendrimer with eight peryleneimide chromophores on the surface and on a monochromophoric model compound is reported. The time-dependent fluorescence spectra of the dendrimer show that the initial excitation is into a locally excited chromophore. They further indicate the existence of a decay channel that leads to excited state interaction between chromophores in one dendrimer which takes place on a 5 ps timescale

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