Nuclear resonant scattering of synchrotron radiation by multilayer structures

Multilayer structures form a particular class of samples employed in nuclear resonant scattering of synchrotron radiation. Their specific properties lead to unusual energy and time characteristics of nuclear resonant scattering, which differ much from those of single crystals. The analysis of these distinctions is presented. Several approaches to achieve pure nuclear reflections with multilayers are discussed. Finally, we review the studies of multilayer structures with nuclear resonant scattering of synchrotron radiation.

     

Enhancement and speedup in nuclear resonant diffraction

The interaction of Mössbauer radiation with the nuclei in a single crystal provides the unique possibility to enhance the coherent channel in nuclear resonance scattering by means of a properly phased excitation of the scattering centers. When a primary beam is incident in the exact Bragg direction, all nuclei are excited in phase. The resonance parameters of such a collective nuclear excitation of a perfect single crystal (γ-exciton) are entirely different from those of an individual nuclear excitation. In Bragg geometry diffraction, the resonance lines are shifted and broadened (enhancement effect), the lifetime of the collective excited state is shortened (speedup effect) and the reflectivity becomes total (suppression effect). Recent experiments arc reviewed, where these effects were studied in the resonant diffraction of Mössbauer and of synchrotron radiation.

     

Basic features of coherent nuclear resonant scattering of synchrotron radiation

The time dependences of spatially coherent nuclear resonant scattering of synchrotron radiation show a wealth of characteristic features which originate from the interference of several radiation components and from dynamical nuclear scattering. These effects will be of importance for the future fields of time domain Mössbauer spectroscopy and of nuclear resonant -ray optics. The basic features are discussed and experimental evidence is reviewed.     

Nuclear resonant scattering of synchrotron radiation

The principal ideas of the theory and the main results of the experimental studies of the coherent resonant scattering of-radiation by nuclear ensembles in matter are briefly over-viewed. An analysis of transmission of the Mössbauer-radiation and of synchrotron radiation through a nuclear resonant medium is suggested using an approach based on the optical theory. The feasibilities of the nuclear resonant scattering of synchrotron radiation as a new technique for studying the hyperfine interactions and some other phenomena of the physics of condensed matter are considered.     

Nuclear resonant scattering using synchrotron radiation

A one-dimensional quantum model for nuclear resonant scattering using synchrotron radiation has been developed. This model gives a clear physical interpretation of the most prominent features of the coherent forward scattering process namely, the “speed-up” and “dynamical beat” effects. The form of the solution, for the time-dependent forward scattered intensity of the resonant radiation from the resonant medium after synchrotron radiation excitation, is a finite series. This unique solution can be interpreted in terms of a summation over all multiple forward scattering paths the radiation takes in reaching the detector. The resonant medium is represented by a linear chain of N effective resonant nuclei. The analysis starts from a coupled set of quantum mechanical equations for the relevant amplitudes in frequency space. Transformation to the time domain gives an analytical expression for the forward scattered intensity. The contribution of every order of the multiple scattering processes from the N effective nuclei appears naturally. The expression gives a clear physical understanding of all relevant aspects of resonant forward nuclear scattering. Furthermore, the present formalism allows the consideration of incoherent processes. This permits the study of processes in which there is gamma emission with recoil or emission of internal-conversion electrons. This revised version was published online in August 2006 with corrections to the Cover Date.     

Polarization effects in resonant nuclear scattering

Polarization phenomena are present in every radiative transition, whether it is of atomic or nuclear origin. Nuclear resonant scattering of synchrotron radiation is an ideal technique for their study because (a) the probing radiation is in a well characterized polarization state, in most cases linear, (b) the scattered radiation can be efficiently analyzed with polarization filters, and (c) synchrotron pulses are very short compared to the lifetime of a nuclear resonance, resulting in a clean signal. In the following article we describe experimental and theoretical studies of the 14.4 keV Mössbauer resonance of ⁵⁷Fe and its transitions with linear and circular polarization. After introducing the required instrumentation a formalism to calculate time dependent polarization phenomena is derived. With the help of different scattering geometries we illustrate various aspects, such as polarization mixing and selective excitation of subsets of the resonance. Perhaps the most fascinating example is the Faraday geometry where the E-vector rotates several 360^ο turns during the lifetime of the resonant scattering. A comparison of this phenomenon with the optical Faraday effect is given. New powerful synchrotron radiation sources will enable researchers to exploit polarization phenomena in nuclear resonant scattering to detect subtle changes in physically and chemically relevant systems.

     

Introduction to nuclear resonant scattering with synchrotron radiation

The concepts leading to the application of synchrotron radiation to elastic and inelastic nuclear resonant scattering are discussed. The resulting new experimental techniques are compared to conventional Mössbauer spectroscopy. A survey of situations that favor experiments with synchrotron radiation is offered.

     

Raman spectra of GaAs-AlxGa1-xAs superlattices

Systematic theoretical studies of Raman spectra of GaAs-Al_xGa_1-xAs superlattices are presented. The electronic states are described by an envelope-function method and the phonon modes are described in a microscopic rigid-ion model. Both resonant and nonresonant Raman scattering processes are considered. For resonant Raman scattering, the effects of discrete exciton states plus the continuum and the valence-band mixing are included via a k-space sampling method. Both the Fröhlich and deformation-potential mechanisms for electron-phonon coupling are considered. These two mechanisms are responsible for principal features in the z(x, x)z̄ and z(x, y)z̄ geometries, respectively. We find that the effects of exciton continuum states are quite important and the resonant Raman spectra so obtained are in much better agreement with experiment compared to those without including the exciton continuum states.     

CONUSS and PHOENIX: Evaluation of nuclear resonant scattering data

Evaluation methods for data obtained by nuclear resonant scattering techniques are discussed. The CONUSS software package for the interpretation of time or energy spectra from coherent elastic nuclear resonant scattering, i.e., forward scattering and Bragg/Laue scattering, is presented. The analysis of phonon spectra obtained by incoherent nuclear resonant scattering is demonstrated using the PHOENIX software.     

High-pressure Mössbauer studies of magnetism in RFe2 Laves phases and Eu-chalcogenides

A review is given on current high-pressure studies of magnetism employing the new method of nuclear forward scattering of synchrotron radiation as well as the conventional Mössbauer effect. Comparative studies of the magnetic properties of intermetallic RFe₂ Laves phases and Eu(II)-chalcogenides are described. We present as examples the pressure induced changes in YFe₂ and ScFe₂ at pressures up to 100 GPa as well as studies of EuTe in the NaCl-type and the CsCl-type high-pressure phase. Future high-pressure applications of nuclear resonant scattering will be discussed.     

Resonant X-ray scattering from a rotating medium: The Nuclear Lighthouse Effect

A coherently excited nuclear state is carried with a rotating sample so that its radiative decay is redirected by the rotation angle that has developed during its lifetime. As a result, the time spectrum of the nuclear decay is mapped to an angular scale. This effect has been observed in nuclear resonant scattering of synchrotron radiation from a rotating ⁵⁷Fe metal foil. Applications with respect to elastic and inelastic nuclear resonant scattering are discussed. This revised version was published online in August 2006 with corrections to the Cover Date.     

Nuclear resonant scattering of synchrotron radiation for the study of dynamics around the glass transition

Motion of ⁵⁷Fe can be observed on a scale of nsec to μsec through nuclear resonant forward scattering of synchrotron radiation. Additional information is obtained by measuring simultaneously incoherent nuclear resonant scattering at nonzero angles. In a glass, one measures the Lamb-Mößbauer factor; in the viscous phase, structural relaxation is observed directly. We apply the method to ferrocene / dibutylphthalate between 140 and 205 K. The mean relaxation times do not follow the observed temperature dependence of other, macroscopic relaxation measurements. We attribute this to a strong wavenumber dependence of the relaxation time. The prospects of nuclear resonant scattering for studying the dynamics of viscous liquids are discussed.     

Waves in resonant random media

Abstract

Electromagnetic properties of resonant inhomogeneous media are investigated. A new type of transverse electromagnetic wave arising due to the effective spatial dispersion is studied. It is shown that scattering on the fluctuations of the resonant frequency of the medium shifts the Cherenkov threshold and reduces the intensity of the Cherenkov radiation.     

同步辐射穆斯堡尔谱学

同步辐射穆斯堡尔谱自从1985年取得突破后, 经历了20多年的长足发展, 已经成为穆斯堡尔谱学的一个成熟的分支。 目前同步辐射穆斯堡尔谱学由两个部分构成: 基于相干核共振散射机制的时域穆斯堡尔谱学和基于非相干非弹性核共振散射机制的X射线谱学。 第三代同步加速器的出现促进了时域穆斯堡尔谱学的发展, 测量得到穆斯堡尔激发态寿命τ期间衰变计数率与时间的关系, 观测到一些有趣的现象。 同步辐射穆斯堡尔谱既能做常规透射谱学研究, 测量各种超精细相互作用及f_LM, δ_SOD等穆斯堡尔参数, 也能利用非弹性核共振散射测量固体的声子谱, 并且也能测出f_LM和 δ_SOD及力常数等, 时域谱和非相干谱的测量精度都高于常规穆斯堡尔谱。 The idea of using synchrotron radiation as a Mössbauer source experienced a breakthrough in 1985, followed by steady development for more than 20 years. Synchrotron Mössbauer spectroscopy consists of two areas. The first one is the so called time domain Mössbauer spectroscopy based on coherent nuclear resonant scattering which permits determination of hyperfine interactions and other Mössbauer parameters such as f_LM and δ_SOD. The other is incoherent nuclear resonant inelastic X ray scattering, which provides vibration information of atoms in a solid, i.e., the phonon density of states. All the experiments have better accuracy than that obtained in conventional Mssbauer spectroscopy.     

Resonant Raman scattering at the indirect exciton in silver bromide

By excitation in the indirect exciton absorption of AgBr at low temperatures selectively enhanced two-phonon Raman scattering is observed. Using different excitation wavelengths the resonance enhancement is found to be associated with the Г-L exciton as intermediate state for the resonant scattering process. The resonant phonons involved are pairs of LA and TA phonons with opposite wave vectors near L. Measurements in the temperature range 2 K ? T ? 40 K show a decrease of the scattering intensity with increasing temperature. The origin of this temperature dependence is due to lifetime broadening of the scattering state. Several features of the indirect exciton absorption of AgBr are discussed.     

Exciton-phonon interaction in mixed silver halides: Resonant Raman scattering vs photoluminescence

An investigation of resonant Raman scattering in mixed crystals of AgBr:Cl at 1.8 K shows that the zero-phonon and LO phonon-assisted exciton luminescence excited in the free indirect exciton absorption, exhibits an anomalous dependence on the exciton photon energy E_L. Close to the exciton gap, the bands show a Raman-like behaviour with their peaks at constant energetic distance from E_L. As E_L is tuned further into the absorption, the bands gradually develop into normal photoluminescence. The effect is explained by taking into account exciton relaxation via scattering by long-wavelength acoustic phonons, a process which is strongly energy dependent. In addition, resonant Raman scattering observed for excitation in the zero-phonon absorption suggests study for the first time of the mode behaviour of certain off-zone center phonons in this system.     

Large electric-field-induced enhancement of resonant Raman scattering of a single quantum well

The electric-field enhancement of the resonant Raman efficiency of confined optical phonon modes in a single quantum well has been observed in an asymmetrical n-type triple-barrier GaAs/AlAs resonant tunneling structure. The measurement takes advantage of an outgoing resonance with the e₂-hh₁ exciton transition confined to the wide quantum well, and according to the polarization properties, the Fröhlich interaction dominates the scattering mechanism. A fifteenfold increase is found from zero field to 7.5 × 10⁴ V/cm, which results from break-down of the parity selection rules for the photon-exciton and the exciton phonon coupling mechanisms.     

How to do resonant nuclear experiments with synchrotron radiation

Summary The use of synchrotron radiation to excite low-lying nuclear resonances is a rapidly developing field showing great promise for hyperfine spectroscopy, phonon spectroscopy and kinetic studies, crystallography, and fundamental physics experiments. Recent technical advances in synchrotron sources, optics, and fast detectors have drastically increased signal rates and expanded the range of samples that can be studied. A typical experiment today uses a high-brightness synchrotron source having X-ray pulses well-separated in time, a meV-bandpass monochromator using perfect crystals of silicon or germanium, a sample containing resonant nuclei, and an avalanche photodiode timing detector. Both coherent and incoherent scattering can be observed; the coherent scattering is used for hyperfine spectroscopy and studies of diffraction interference phenomena, and the incoherent-scattering signal promises to be very useful for phonon spectroscopy and other studies of excitations in condensed systems. At this point seven nuclear isotopes have been used to resonantly scatter synchrotron radiation, but the number is rapidly increasing. Paper presented at the ICAME-95, Rimini 10–16 September 1995.     

Coherent response of a semiconductor microcavity in the strong coupling regime

We have studied the coherent dynamics of a semiconductor microcavity by means of interferometric correlation measurements with subpicosecond time resolution in a backscattering geometry. Evidence is brought of the resolution of a homogeneous polariton line in an inhomogeneously broadened exciton system. Surprisingly, photon-like polaritons exhibit an inhomogeneous dephasing. Moreover, we observe an unexpected stationary coherence up to 8 ps for the lower polariton branch close to resonance. All these experimental results are well reproduced within the framework of a linear dispersion theory assuming a coherent superposition of the reflectivity and resonant Rayleigh scattering signals with a well-defined relative phase.     

Polarization of photons emitted in the process of resonant coherent excitation of relativistic ions under planar channeling conditions

Owing to the recent observation of the strong anisotropy of characteristic X-ray radiation accompanying the resonant coherent excitation of relativistic Fe²⁴⁺ ions under planar channeling conditions in a silicon crystal, the resonant coherent excitation method can be considered as a candidate for a source of polarized X-ray radiation. The Stokes parameters of the radiation have been calculated using the density matrix approach. The behavior of the polarization characteristics of the radiation in various directions has been explained by considering the properties of the resonance part of the crystal field, which excites an ion and has the form of an elliptically polarized electric field.