First observation of nonreciprocal X-Ray gyrotropy

We report the first observation of a nonreciprocal x-ray linear dichroism caused by the time-reversal odd, real part zeta of the complex gyrotropy tensor zeta(*) which is dominated by electric dipole-electric quadrupole E1E2 interference terms. A nonreciprocal transverse anisotropy was observed in the low temperature insulating phase of a Cr doped V2O3 Mott crystal when a single antiferromagnetic domain was grown by magnetoelectric annealing along the hexagonal c axis. This new element (edge) specific spectroscopy could nicely complement x-ray magnetic circular dichroism which is silent for antiferromagnetic materials.

Element-selective X-ray detected magnetic resonance: a novel application of synchrotron radiation.

X-ray detected magnetic resonance (XDMR) is a new element-selective spectroscopy in which X-ray magnetic circular dichroism is used to probe the resonant precession of spin and orbital magnetization components when a strong microwave pump field is applied perpendicularly to the static bias field. Experimental configurations suitable for detecting the very weak XDMR signal are compared. XDMR signatures were measured in yttrium iron garnet and related thin films on exciting not only the iron K-edge but also the yttrium at diamagnetic sites. These measurements are shown to yield unique information regarding the wide-angle precession of induced magnetization components involving either orbital p-projected densities of states at the iron sites, or spin polarized d-projected densities of states at the yttrium sites. Extending XDMR measurements into the millimeter wave range would make it possible to study paramagnetic systems routinely and investigate optical modes as well as acoustic modes in ferrimagnetic/antiferromagnetic systems.

Advanced detection systems for X-ray fluorescence excitation spectroscopy.

This paper accounts for selected detector developments carried out over the past 15 years within the ESRF X-ray Absorption Spectroscopy group. This includes various types of photodiodes used as integrated current detectors. Special emphasis is put on the long-standing development of a Si drift-diode array suitable for energy-dispersive detection of X-ray fluorescence. This detector, which is now operational, was used to record high-quality XMCD/XAFS spectra on [Fe70Pt30] nanoparticles highly dispersed on a Si wafer. Using numerically deconvoluted spectra, energy resolution was decreased to 82 eV for the Si Kalphabeta line, 126 eV for the Fe Kalpha line and 176 eV for the Pt Lalpha line. A high-vacuum-compatible high-energy-resolution crystal analyzer was also installed on ID12, making it possible to record X-ray fluorescence excitation spectra in the photon-in/photon-out mode over a wide spectral range. Prospects of adapting these methods in order to investigate biological samples are briefly discussed.

Multi-segmented piezoelectric mirrors as active/adaptive optics components.

The angular acceptance of piezoelectric (Pzt) bimorph mirrors is limited by the maximum length of commercially available Pzt ceramic plates. To overcome this limit and manufacture longer devices, several (2n + 1) 150 mm-long bimorph Pzt stacks were assembled side-to-side. Two prototype mirrors, 450 (n = 1) and 750 (n = 2) mm long, were designed, assembled, polished and optically characterized. They are fully UHV compatible and are now installed in the monochromatic section of the ESRF beamlines ID26 and ID32. Both mirrors cover the full range of required bending radii (1 km concave-3.5 km convex). Junctions between segments do not spoil the optical surface quality. The surface slope error r.m.s. can be kept well below 1 arcsec over the full bending range. Adaptive compensation for low-frequency figure errors was shown to be easy and reliable. After compensation, residual shape errors are of the order of 40 nm r.m.s. over 700 mm.

X-ray natural circular dichroism and chiral-EXAFS in gyrotropic crystals.

X-ray natural circular dichroism (XNCD) has been recently detected in the XANES region for uniaxial and biaxial gyrotropic crystals. Chiral-EXAFS (chi-EXAFS) spectra are reported for the first time over a wider energy range and are analysed in terms of multiple-scattering paths of relevant symmetry. For such heavily absorbing single crystals as lithium iodate, paratellurite or potassium titanyl phosphate, the differential absorption between left-handed and right-handed circularly polarized X-ray photons cannot be measured in transmission but gyrotropy effects can still be detected in fluorescence excitation spectra. Whereas XNCD and fluorescence-detected X-ray natural circular dichroism spectra are strictly identical for uniaxial crystals, it has been established that this was true only to the first order for biaxial crystals such as potassium titanyl phosphate.

XAFS and X-MCD spectroscopies with undulator gap scan.

The first experimental applications of the undulator gap-scan technique in X-ray absorption spectroscopy are reported. The key advantage of this method is that during EXAFS scans the undulator is permanently tuned to the maximum of its emission peak in order to maximize the photon statistics. In X-MCD or spin-polarized EXAFS studies with a helical undulator of the Helios type, the polarization rate can also be kept almost constant over a wide energy range.

X-ray magnetic reflectometry using circularly polarized radiation.

Magnetic reflectometry experiments have been performed in the X-ray range at the L(2,3) edges of rhodium. What makes these experiments original is the insertion of a very compact double-bounce reflectometer upstream of the monochromator. This configuration makes full use of the high polarization rate of the helical undulator source. This advantage is reflected in the high quality of the data obtained after only a few accumulations. It is also shown that, by properly selecting the angle of incidence, one may obtain experimental differential X-ray reflectivity spectra dominated either by the dispersion or the absorption terms.

Design of an X-ray Phase-Plate Analyzer to Measure the Circular Polarization Rate of a Helical Undulator Source.

A quarter-wave plate made of a ca 16 mum-thick silicon single-crystal was used at energies as low as 2.8 keV to convert circularly polarized photons into linearly polarized photons. Coupled to a linear polarimeter, this quarter-wave plate enabled the characterization of the circular polarization rate of the radiation emitted by one of the ESRF helical undulators, Helios-I. The measured value (ca 97%) is in good agreement with theoretical predictions. Special attention was paid to the alignment procedures of all relevant optical components of the beamline.

X-ray magnetochiral dichroism: a new spectroscopic probe of parity nonconserving magnetic solids.

We report the first experimental detection of x-ray magnetochiral dichroism in magnetoelectric Cr2O3. This dichroism, which does not require any polarized x-ray beam, is related to the time-reversal odd part of the optical activity tensor dominated by electric dipole-electric quadrupole E1E2 interference terms. The experiments were carried out using either a single crystal or a powdered pellet required to grow a single antiferromagnetic domain by magnetoelectric annealing. This new element (edge) specific spectroscopy offers unique access to the atomic orbital anapole moment Omega-z.

Natural linear dichroism in pyrite (FeS2): experiments and calculations.

Electric quadrupole transitions are revealed through the angular dependence of X-ray absorption spectra in a cubic crytal. Data collection was achieved at the iron K-edge in pyrite (FeS2) by using the angular moment method developed for X-ray Natural Circular Dichoism (XNCD) measurements. The natural linear dichroism (XNLD) was found to be around 0.5% of the edge jump. Experimental results are compared with monelectronic and multilectronic calculations. Calculations allow to quantitatively determine the proportion of quadrupolar transitions in the pre-edge structure and the anisotropy is explained in terms of structural and electronic parameters.

Development of 32-channel silicon drift detectors and digital electronics for X-ray spectroscopy.

The performance of silicon-drift-detector (SDD) arrays and digital electronics designed for X-ray absorption spectroscopy in the fluorescence excitation mode is reported. Different detectors have been manufactured and tested: two single-channel SDDs with different active areas (10 mm(2) and 1 cm(2)) and a monolithic 2 cm(2) SDD with eight readout anodes. The energy resolution varies between 160 and 170 eV FWHM. A new digital multichannel shaping amplifier has been produced. Its performance is presented in comparison with that of a standard commercial shaper.

Instrumentation Developments for X-ray Linear and Circular Dichroism at the ESRF Beamline ID12A.

This paper reports on the performance of the instrumentation developed for the ESRF beamline ID12A, which is dedicated to spectroscopic applications requiring full control of the polarization at energies >/=2.0 keV. Emphasis is placed on the characterization of various optical components of the beamline and on problems associated with either the control or the conversion of the polarization state. A few examples have been selected to illustrate what sort of new spectroscopic information has already been obtained at the beamline. These include the comparison of X-ray magnetic dichroism spectra recorded with linear or circular polarization and the very first detection of X-ray natural circular dichroism in single crystals known to exhibit a very large non-linear susceptibility at optical wavelengths.