Biomedical subjects

W Sturhahn

Publications and source records attributed to W Sturhahn.

At least 19 recordsLinked to original sources

PubMed2006

A cryogenically stabilized meV-monochromator for hard X-rays.

The design and performance results for a cryogenically stabilized high-resolution monochromator for 23.880 keV (lambda = 52 pm) X-rays are presented. The four-crystal-reflection monochromator is suitable for nuclear resonant scattering measurements from 119Sn compounds using synchrotron radiation. The design includes a low-vibration cryostat that maintains two of the four crystal reflections at a temperature where the coefficient for thermal expansion of the crystalline material (silicon) vanishes. Test results demonstrate a 1.3 meV bandwidth with negligible broadening due to vibrations and a spectral efficiency of 37% when used with an undulator source.

Journal Article↗

PubMed2005

Anharmonic motions of Kr in the clathrate hydrate.

The anomalous glass-like thermal conductivity of crystalline clathrates has been suggested to be the result of the scattering of thermal phonons of the framework by 'rattling' motions of the guests in the clathrate cages. Using the site-specific (83)Kr nuclear resonant inelastic scattering spectroscopy in combination with conventional incoherent inelastic neutron scattering and molecular-dynamics simulations, we provide unambiguous evidence and characterization of the effects on these guest-host interactions in a structure-II Kr clathrate hydrate. The resonant scattering of phonons led to unprecedented large anharmonic motions of the guest atoms. The anharmonic interaction underlies the anomalous thermal transport in this system. Clathrates are prototypical models for a class of crystalline framework materials with glass-like thermal conductivity. The explanation of the unusual molecular dynamics has a wide implication for the understanding of the thermal properties of disordered solids and structural glasses.

Computer Simulation↗

PubMed2004

Nuclear resonant magnetometry and its application to Fe/Cr multilayers.

We introduce nuclear resonant magnetometry as a means to record the magnetization curve of isotopically enhanced regions of a sample. It is based on nuclear resonant scattering with circularly polarized synchrotron radiation and the use of a nuclear resonant reference sample. We apply this approach to study the interlayer coupling in Fe/Cr(100) multilayers and to obtain a layer-specific magnetization curve. Our measurements provide experimental evidence for the existence of a nontrivial interlayer-coupling angle in Fe/Cr/Fe.

Journal Article↗

PubMed2002

Vibrational dynamics of myoglobin determined by the phonon-assisted Mössbauer effect.

The phonon-assisted Mössbauer effect is used to determine the partial phonon density of states of the iron within the active center of deoxymyoglobin, carboxymyoglobin, and dry and wet metmyoglobin between 40 and 300 K. Between 0 and 1 meV the iron density of states increases quadratically with the energy, as in a Debye solid. Mean sound velocities are extracted from this slope. Between 1 and 3 meV a nearly quadratic "Debye-like" increase follows due to the similar strength of intermolecular and intramolecular forces. Above 3 meV, optical vibrations are characteristic for the iron-ligand conformation. The overall mean square displacements of the heme iron atom obtained from the density of states agree well with the values of Mössbauer absorption experiments below 180 K. In the physiological temperature regime the data confirm the existence of harmonic vibrations in addition to the protein specific dynamics measured by Mössbauer absorption. In the Debye energy regime the mean square displacement of the iron is in agreement with that of the hydrogens measured by incoherent neutron scattering demonstrating the global character of these modes. At higher energies the vibration of the heavy iron atom at 33 meV in metmyoglobin is as large as that of the lightweight hydrogens at that energy. A freeze dried, rehydrated (h=0.38 g H2O/g protein) metmyoglobin sample shows an excess of states above the Debye law between 1 and 3 meV, similar to neutron scattering experiments. The room temperature density of states below 3 meV exhibit an increase of the density compared to the low temperature data, which can be interpreted as mode softening.

Journal Article↗

PubMed2001

Nuclear inelastic x-ray scattering of FeO to 48 GPa.

The partial density of vibrational states has been measured for Fe in compressed FeO (wüstite) using nuclear resonant inelastic x-ray scattering. Substantial changes have been observed in the overall shape of the density of states close to the magnetic transition around 20 GPa from the paramagnetic (low pressure) to the antiferromagnetic (high pressure) state. The results indicate that strong magnetoelastic coupling in FeO is the driving force behind the changes in the phonon spectrum of FeO. The paper presents the first observation of changes in the density of terahertz acoustic phonon states under magnetic transition at high pressure.

Journal Article↗

PubMed2001

Observation of the 22.5-keV resonance in (149)Sm by the nuclear lighthouse effect.

We have observed coherent nuclear resonant scattering of synchrotron radiation at the 22.5-keV resonance of (149)Sm. High-speed rotational sample motion led to an angular deflection of the resonantly scattered radiation off the nonresonant primary beam. This allowed us to determine the resonance energy of the first excited nuclear level of (149)Sm to be 22496(4) eV. Because of the angular deflection of the resonant photons, time spectra of coherent nuclear resonant scattering can be recorded as a function of a spatial coordinate. Time resolutions of a few 10 ps can be expected, which are beyond the limits of existing x-ray detection schemes.

Journal Article↗

PubMed2001

Crystal monochromator with a resolution beyond 10(8).

Monochromatization with crystal diffraction has been achieved to a resolution (lambda/delta lambda) beyond 10(8). The monchromator is specifically designed for 23.880 keV synchrotron radiation (lambda = 51.9 pm) for applications involving nuclear resonant scattering from 119Sn. The design uses asymmetrically cut silicon (12 12 12) crystal reflections from two single-crystalline monoliths oriented in a dispersive geometry. A transmitted energy bandwidth of 140 +/- 20 mu eV was measured, corresponding to a resolution of 1.7 x 10(8). Methods of improving efficiency, wavelength stability and resolution are discussed.

Journal Article↗

PubMed2001

Long-range reactive dynamics in myoglobin.

We report the complete vibrational spectrum of the probe nucleus 57Fe at the oxygen-binding site of the protein myoglobin. The Fe-pyrrole nitrogen stretching modes of the heme group, identified here, probe asymmetric interactions with the protein environment. Collective oscillations of the polypeptide, rather than localized heme vibrations, dominate the low frequency region. We conclude that the heme "doming" mode is significantly delocalized, so that distant sites respond to oxygen binding on vibrational time scales. This has ramifications for understanding long-range interactions in biomolecules, such as those that mediate cooperativity in allosteric proteins.

Animals↗

PubMed2001

Phonon density of states of iron up to 153 gigapascals.

We report phonon densities of states (DOS) of iron measured by nuclear resonant inelastic x-ray scattering to 153 gigapascals and calculated from ab initio theory. Qualitatively, they are in agreement, but the theory predicts density at higher energies. From the DOS, we derive elastic and thermodynamic parameters of iron, including shear modulus, compressional and shear velocities, heat capacity, entropy, kinetic energy, zero-point energy, and Debye temperature. In comparison to the compressional and shear velocities from the preliminary reference Earth model (PREM) seismic model, our results suggest that Earth's inner core has a mean atomic number equal to or higher than pure iron, which is consistent with an iron-nickel alloy.

Journal Article↗

PubMed2000

Wavelength-dispersive double flat-crystal analyzer for inelastic X-ray scattering.

A double flat-crystal analyzer for inelastic X-ray scattering is described. The general correlation between the energy and direction of the X-rays transmitted by the analyzer allows one to collect data for a range of energy transfers simultaneously. Such an analyzer with 120 meV resolution was built to operate at the copper K edge. Experimental results show that this X-ray optic can be an alternative to a conventional spherical-focusing backscattering analyzer in resonant inelastic X-ray scattering experiments or when flexible energy resolution or high momentum resolution is required.

Journal Article↗

PubMed2000

gamma-Ray wavelength standard for atomic scales.

The wavelength of the 57Fe Mössbauer radiation is measured with a relative uncertainty of 0.19 ppm by using almost exact Bragg backscattering from a reference silicon crystal. Its value is determined as lambda(M) = 0.860 254 74(16)x10(-10) m. The corresponding Mössbauer photon energy is E(M) = 14 412.497(3) eV. The wavelength of the 57Fe Mössbauer radiation is easily reproducible with an accuracy of at least 10(-11)lambda(M) and could be used as a length standard of atomic dimensions.

Journal Article↗

PubMed2000

Coherent resonant x-ray scattering from a rotating medium.

A coherently excited nuclear state in a rotating sample acquires a phase shift during its time evolution that is proportional to its angular momentum and the rotation angle. As a consequence, the radiative decay of the excited state proceeds into the rotated direction, and the time spectrum of the nuclear decay is mapped onto an angular scale. This effect has been observed in nuclear resonant scattering of synchrotron radiation from a 57Fe metal foil rotating at 18 kHz.

Journal Article↗

PubMed2000

Nuclear forward scattering of synchrotron radiation by deoxymyoglobin.

Nuclear forward scattering of synchrotron radiation is used to determine the quadrupole splitting and the mean square displacement of the iron atom in deoxymyoglobin in the temperature range between 50 K and 243 K. Above 200 K an abnormally fast decay of the forward scattered intensity at short times after the synchrotron flash is observed, which is caused by protein-specific motions. The results strongly support the picture that protein dynamics seen at the position of the iron can be understood by harmonic motions in the low temperature regime while in the physiological regime diffusive motions in limited space are present. The shape of the resonance broadening function is investigated. An inhomogeneous broadening with a Lorentzian distribution indicating dipole interactions results in a better agreement with the experimental data than the common Gaussian distribution.

Animals↗

PubMed1996