Aleksandr I. Chumakov

Experimental aspects of inelastic nuclear resonance scattering

We present an introduction to the technique of inelastic nuclear scattering. The details of experimental setup, instrumentation, and measuring procedure are discussed. The typical appearance of experimental results and a brief description of data treatment methods are illustrated by examples of recent studies. Finally, the scope of information on lattice dynamics that is accessible with inelastic nuclear scattering is outlined.

The 57Fe Synchrotron Mössbauer Source at the ESRF.

The design of a (57)Fe Synchrotron Mössbauer Source (SMS) for energy-domain Mössbauer spectroscopy using synchrotron radiation at the Nuclear Resonance beamline (ID18) at the European Synchrotron Radiation Facility is described. The SMS is based on a nuclear resonant monochromator employing pure nuclear reflections of an iron borate ((57)FeBO(3)) crystal. The source provides (57)Fe resonant radiation at 14.4 keV within a bandwidth of 15 neV which is tunable in energy over a range of about ±0.6 µeV. In contrast to radioactive sources, the beam of γ-radiation emitted by the SMS is almost fully resonant and fully polarized, has high brilliance and can be focused to a 10 µm × 5 µm spot size. Applications include, among others, the study of very small samples under extreme conditions, for example at ultrahigh pressure or combined high pressure and high temperature, and thin films under ultrahigh vacuum. The small cross section of the beam and its high intensity allow for rapid collection of Mössbauer data. For example, the measuring time of a spectrum for a sample in a diamond anvil cell at ∼100 GPa is around 10 min, whereas such an experiment with a radioactive point source would take more than one week and the data quality would be considerably less. The SMS is optimized for highest intensity and best energy resolution, which is achieved by collimation of the incident synchrotron radiation beam and thus illumination of the high-quality iron borate crystal within a narrow angular range around an optimal position of the rocking curve. The SMS is permanently located in an optics hutch and is operational immediately after moving it into the incident beam. The SMS is an in-line monochromator, i.e. the beam emitted by the SMS is directed almost exactly along the incident synchrotron radiation beam. Thus, the SMS can be easily utilized with all existing sample environments in the experimental hutches of the beamline. Owing to a very strong suppression of electronic scattering for pure nuclear reflections (∼10(-9)), SMS operation does not required any gating of the prompt electronic scattering. Thus, the SMS can be utilized in any mode of storage ring operation.

Vibrational spectrum of the spin crossover complex [Fe(phen)2(NCS)2] studied by IR and Raman spectroscopy, nuclear inelastic scattering and DFT calculations

The vibrational modes of the low-spin and high-spin isomers of the spin crossover complex [Fe(phen)(2)(NCS)(2)] (phen = 1,10-phenanthroline) have been measured by IR and Raman spectroscopy and by nuclear inelastic scattering. The vibrational frequencies and normal modes and the IR and Raman intensities have been calculated by density functional methods. The vibrational entropy difference between the two isomers, DeltaS(vib), which is--together with the electronic entropy difference DeltaS(el)--the driving force for the spin-transition, has been determined from the measured and from the calculated frequencies. The calculated difference (DeltaS(vib) = 57-70 J mol(-1) K(-1), depending on the method) is in qualitative agreement with experimental values (20-36 J mol(-1) K(-1)). Only the low energy vibrational modes (20% of the 147 modes of the free molecule) contribute to the entropy difference and about three quarters of the vibrational entropy difference are due to the 15 modes of the central FeN(6) octahedron.

Portable laser‐heating system for diamond anvil cells

The diamond anvil cell (DAC) technique coupled with laser heating has become the most successful method for studying materials in the multimegabar pressure range at high temperatures. However, so far all DAC laser-heating systems have been stationary: they are linked either to certain equipment or to a beamline. Here, a portable laser-heating system for DACs has been developed which can be moved between various analytical facilities, including transfer from in-house to a synchrotron or between synchrotron beamlines. Application of the system is demonstrated in an example of nuclear inelastic scattering measurements of ferropericlase (Mg(0.88)Fe(0.12))O and h.c.p.-Fe(0.9)Ni(0.1) alloy, and X-ray absorption near-edge spectroscopy of (Mg(0.85)Fe(0.15))SiO(3) majorite at high pressures and temperatures. Our results indicate that sound velocities of h.c.p.-Fe(0.9)Ni(0.1) at pressures up to 50 GPa and high temperatures do not follow a linear relation with density.

Effect of iron oxidation state on the electrical conductivity of the Earth’s lower mantle

Iron can adopt different spin states in the lower mantle. Previous studies indicate that the dominant lower-mantle phase, magnesium silicate perovskite (which contains at least half of its iron as Fe(3+)), undergoes a Fe(3+) high-spin to low-spin transition that has been suggested to cause seismic velocity anomalies and a drop in laboratory-measured electrical conductivity. Here we apply a new synchrotron-based method of Mössbauer spectroscopy and show that Fe(3+) remains in the high-spin state in lower-mantle perovskite at conditions throughout the lower mantle. Electrical conductivity measurements show no conductivity drop in samples with high Fe(3+), suggesting that the conductivity drop observed previously on samples with high Fe(2+) is due to a transition of Fe(2+) to the intermediate-spin state. Correlation of transport and elastic properties of lower-mantle perovskite with electromagnetic and seismic data may provide a new probe of heterogeneity in the lower mantle.

Density of phonon states in superconducting FeSe as a function of temperature and pressure

The temperature and pressure dependence of the partial density of phonon states (phonon-DOS) of iron atoms in superconducting

Nuclear inelastic scattering

{\text{Fe}}_{1.01}\text{Se}

Structural complexity of simple Fe2O3 at high pressures and temperatures

was studied by

High-energy-resolution x-ray optics with refractive collimators

^{57}\text{F}\text{e}

Insight to Dynamics of Molecules with Nuclear Inelastic Scattering

nuclear inelastic scattering. The high-energy resolution allows for a detailed observation of spectral properties. A sharpening of the optical phonon modes and shift of all spectral features toward higher energies by