Technical Report: In-situ Monitoring and Validation of a Uranium Mill Tailings Management Facility Design Using X-ray Absorption Near Edge Structure (XANES) Spectroscopy

SOLEIL, a 2.75 GeV third-generation synchrotron light source [1 Nadji, A., Brunelle, P., Couprie, M.-E., Denard, J.-C., Filhol, J.-M., Lamarre, J.-F., Lebasque, P., Loulergue, A., Marchand, P., Nagaoka, R. and Nadolski, L. S. Proceedings of the Second International Particle Accelerator Conference. San Sebastian, Spain. pp.3002–3004.  [Google Scholar]], is presently delivering photons to 24 beamlines for users in five different filling patterns with top-up injection. The 430 mA multibunch (with three successive quarters filled; i.e., 312 out of 416 bunches) is complemented with time-resolved (hybrid multibunch, eight bunches and single bunch) and 4-2 ps bunch-length low-alpha modes. Even shorter bunches will be available at the end of 2013 with the forthcoming Femto-slicing project. With the continuous improvements of transverse beam position (200 nm RMS in the vertical plane) and the understanding of collective effects, the beam current and the stability provided to the beamlines have been steadily increased. New exotic modes of operation and upgrades of the optics to reduce the 3.9 nm.rad horizontal emittance are being studied.     

Looking Deeper: Angle-Resolved Photoemission with Soft and Hard X-rays

Traditional angle-resolved photoemission (ARPES) with excitation in the ca. 20 to 150 eV range has clearly evolved to be the technique of choice for studying the electronic structure of surfaces and complex new strongly correlated and magnetic materials. However, it is clear that ARPES with excitation only up to 150 eV or so remains a very surface-sensitive probe, thus necessitating careful in-situ sample treatment, cleaving, or even synthesis to avoid the measurement of surface-associated artifacts. A key measure of this surface sensitivity is the electron inelastic mean free path (IMFP orΛ_e), which measures the mean depth of electron emission without inelastic scattering, and both experimental [1 Offi, F., Iacobucci, S., Vilmercati, P., Rizzo, A., Goldoni, A., Sacchi, M. and Panaccione, G. 2008. Physical Review B, 77: 201101R[Crossref] , [Google Scholar], 2 Offi, F., Iacobucci, S., Petaccia, L., Gorovikov, S., Vilmercati, P., Rizzo, A., Ruocco, A., Goldoni, A., Stefani, G. and Panaccione, G. 2010. Journal of Physics: Condensed Matter, 22: 305002[Crossref] , [Google Scholar]] and theoretical [3 Tanuma, S., Powell, C. J. and Penn, D. R. 2011. Surface and Interface Analysis, 43: 689[Crossref], [Web of Science ®] , [Google Scholar]] IMFP studies showing that the only reliable way to increase bulk or buried layer/interface sensitivity for all material types is to go to higher photon energies in the soft X-ray (ca. 0.5–2 keV) or hard X-ray (ca. 2–10 keV) regime.     

Boundary conditions for phase transitions and interfacial reactions

Abstract

Si et al. [1 Si, X., Oh, E.S. and Slattery, J.C. 2010. Phil. Mag., 90: 655[Taylor & Francis Online] , [Google Scholar]] pointed out that it was inappropriate to use continuity of displacement at interfaces during phase transitions or in the case of reactions at interfaces as in the case of oxidation, since appropriate reference configurations cannot be identified. They instead derived a new compatibility constraint, when atleast one of the adjoining phases is crystalline. The test of these ideas offered by Slattery et al. [2 Slattery, J.C., Si, X., Fu, K.B. and Oh, E.S. 2010. Phil. Mag., 90: 665[Taylor & Francis Online] , [Google Scholar]] was successful, but it likely was too simple, since the deformations were so small. A more stringent and successful test has recently been offered by [3 Slattery, J.C., Fu, K-B and Philos, E-SOh. 2012. Mag., 92: 1788 [Google Scholar]]. Here, we analyze oxidation on the surface of a cylinder both using an extension of the compatibility constraint and using continuity of displacement, comparing the results with the experimental observations of Imbrie and Lagoudas [4 Imbrie, P.K. and Lagoudas, D.C. 2001. Oxid. Met., 55: 359[Crossref], [Web of Science ®] , [Google Scholar]].     

Laser-Seeded Free-Electron Lasers at the NSLS

The National Synchrotron Light Source (NSLS) has a long tradition of research and development in accelerator physics and light source technologies. Over the past two decades, the NSLS has made many pioneering contributions to the development of storage-ring-based light sources, such as the Chasman-Green lattice, global orbit feedback systems, and in-vacuum insertion devices. Even from the earliest days of the NSLS, the staff also had started to explore the potential of free-electron-laser (FEL)-based light sources, leading to some seminal work on the theory of self amplified spontaneous emission (SASE) FELs [1 Bonifacio, R., Pellegrini, C. and Narducci, L. 1984. Optics Comm., : 373 [Google Scholar],2 Wang, J.M. and Yu, L.H. 1986. NIM A, 250: 484 [Google Scholar]].     

Low-temperature high-resolution absorption spectrum of 14NH3 in the ν1+ν3 band region (1.51 μm)

Jet-cooled spectra of ¹⁴NH₃ and ¹⁵NH₃ in natural abundance were recorded using cavity ring-down (CRDS, 6584–6670 cm^?1) and cavity enhanced absorption (CEAS, 6530–6700 cm^?1) spectroscopy. Line broadening effects in the CRDS spectrum allowed lines with J ^″-values between 0 and 3 to be identified. Intensity ratios in ¹⁴NH₃ between the jet-cooled CRDS and literature room-temperature data from Sung et al. (J. Quant. Spectrosc. Radiat. Transfer, 113 (2012 K. Sung , L.R. Brown , X. Huang , D.W. Schwenke , T.J. Lee , S.L. Coy , and K.K. Lehmann , J. Quant. Spectrosc. Radiat. Transfer 113 , 1066 (2012).[Crossref], [Web of Science ®] , [Google Scholar]), 1066) further assisted the line assignments. Ground state combination differences were extensively used to support the assignments, providing reliable values for J, K and inversion symmetry of the ground state vibrational levels. CEAS data helped in this respect for the lowest J lines, some of which are saturated in the CRDS spectrum. Further information on a/s doublets arose from the observed spectral structures. Thirty-two transitions of ¹⁴NH₃ were assigned in this way and a limited but significant number (19) of changes in the assignments results, compared to Sung et al. or to Cacciani et al. (J. Quant. Spectrosc. Radiat. Transfer, 113 (2012 P. Cacciani , P. Cermak , J. Cosleou , M. Khelkhal , P. Jeseck , and X. Michaut , J. Quant. Spectrosc. Radiat. Transfer 113 , 1084 (2012).[Crossref], [Web of Science ®] , [Google Scholar]), 1084). Sixteen known and 25 new low-J transitions were identified for ¹⁵NH₃ in the CRDS spectrum but the much scarcer literature information did not allow for any more refined assignment. The present line position measurements improve on literature values published for ¹⁵NH₃ and on some line positions for ¹⁴NH₃.     

LURE in the 1970s

In France, Yvette Cauchois, Director of the Laboratoire de Chimie Physique in Paris, was the first person who came up with the idea of using synchrotron radiation. The experiment was done in collaboration with Italian scientists at the Frascati synchrotron in 1963 [1 Y. Cauchois, C. Bonnelle and G. Missoni, C. R. Acad. Sci. Paris, 257, 409 (1963a) and 1242 (1963b). [Google Scholar]]. For a few years, interesting results were obtained by her group and that of Pierre Jaéglé (Orsay) [2 P. Jaeglé, P. Missoni and P. Dhez, Phys. Rev. Lett., 18, 887 (1967).[Crossref], [Web of Science ®] , [Google Scholar]]. After that, they contacted the laboratory for high-energy physics at Orsay (LAL), hoping to install a beamline on the ACO (electron-positron collider), but their request was turned down.     

The pseudogap: friend or foe of high T c ?

Although nineteen years have passed since the discovery of high temperature cuprate superconductivity 1 Bednorz, JG and Müller, KA. 1986. Z. Phys. B, 64: 189[Crossref] , [Google Scholar], there is still no consensus on its physical origin. This is in large part because of a lack of understanding of the state of matter out of which the superconductivity arises. In optimally and underdoped materials, this state exhibits a pseudogap at temperatures large compared to the superconducting transition temperature 2 Warren, WW Jr., Walstedt, RE, Brennert, GF, Cava, RJ, Tycko, R, Bell, R and Dabbagh, G. 1989. Phys. Rev. Lett., 62: 1193[Crossref], [PubMed], [Web of Science ®] , [Google Scholar], 3 Alloul, H, Ohno, T and Mendels, P. 1989. Phys. Rev. Lett., 63: 1700[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]. Although discovered only three years after the pioneering work of Bednorz and Müller, the physical origin of this pseudogap behavior and whether it constitutes a distinct phase of matter is still shrouded in mystery. In the summer of 2004, a band of physicists gathered for five weeks at the Aspen Center for Physics to discuss the pseudogap. In this perspective, we would like to summarize some of the results presented there and discuss the importance of the pseudogap phase in the context of strongly correlated electron systems.

The pseudogap: friend or foe of high T _c ?

All authors

M. R. Norman, D. Pines &; C. Kallin

https://doi.org/10.1080/00018730500459906

Published online:

19 February 2007

Table     

Thermodynamics of two-dimensional single-component elastic crystalline solids: single-wall carbon nanotubes

The thermodynamic behaviour of two-dimensional single-component elastic crystalline solids is developed: the surface Euler's equation, the surface Gibbs equation, the surface Gibbs–Duhem equation, and the conditions to be expected at equilibrium, including the stress-deformation behaviour of the crystal. The analysis recognizes that the surface Helmholtz free energy is an explicit function of the lattice vectors defining the crystalline structure. As an application, we obtain the stress-deformation behaviour of single-wall carbon nanotubes which are composed of a regular two-dimensional array of hexagonal lattices of carbon atoms. Using two potentials, Tersoff [1] Tersoff J Phys. Rev. B 37 6991 1988 [Crossref], [Web of Science ®] , [Google Scholar]–Brenner [2] Brenner DW Phys. Rev. B 42 9458 1990 [Crossref], [Web of Science ®] , [Google Scholar] and Brenner et al. [3] Brenner, DW, Shenderova, OA, Harrison, JA, Stuart, SJ, Ni, B and Sinnott, SB. 2002. J. Phys. Condens. Matter, 14: 783[Crossref], [Web of Science ®] , [Google Scholar] to describe interatomic potentials and hence the specific surface Helmholtz free energy, we compute the surface elastic properties for the single-wall carbon nanotubes. These are compared with the available experimental values.     

Magnetic Measurement Techniques for the Large-Scale Production of Undulator Segments for the European XFEL

The European X-ray free electron laser (EXFEL) facility is currently under construction [1 M. Altarelli, The European X-ray Free-electron Laser, Technical Design Report (2006). [Google Scholar]]. Using the principle of self-amplified spontaneous emission (SASE) [2 A.M. Kondratenko and E.L. Saldin, Part. Accel., 10, 207 (1980). [Google Scholar], 3 R. Bonifacio, C. Pellegrini, and L.M. Narducci, Opt. Commum. 50, 373 (1984).[Crossref], [Web of Science ®] , [Google Scholar]], intense FEL radiation is generated in three gap-tuneable undulator systems called SASE1, SASE2, and SASE3. The electron beam energy of the EXFEL is variable between 8.5 and 17.5 GeV. SASE1 and SASE2 are hard X-ray FELs using planar undulators with a period length of 40 mm, called U40s. By a suitable choice of the beam energy and undulator gap, the wavelength can be tuned from 0.05 to 0.4 nm. SASE3 is a soft X-ray FEL using planar undulators with a period length of 68 mm, called U68s. Under the same conditions, the wavelength can be tuned from 0.4 to 5.2 nm.     

Future light sources based upon photo-injected energy recovery linacs

X-ray scattering techniques have long ranked among the most important methods for studying amorphous materials and other highly disordered targets. Well-established X-ray scattering methods often consist of recording time-averaged scattered intensity maps which, under the Born approximation, straightforwardly reveal information about ensemble-averaged, two-point, electron density correlations within the target. In the case of isotropic targets that consist of disordered ensembles of randomly oriented particles, scattering data are typically reduced to a histogram of electron pair distances (the “pair distribution function,” or PDF). While the information contained in the one-dimensional PDF is limited, a rich set of structural properties can often be determined straightforwardly (e.g., radius of gyration, surface area, short-range correlation length scales, fractal dimension). One of the well-known pinnacles of the methodology is the application of small-angle X-ray scattering (SAXS) to solutions of identical biological macromolecules [1 Elser, V. 2011. New J. Phys., 13: 123014[Crossref] , [Google Scholar]–3 Putnam, C. D., Hammel, M., Hura, G. L. and Tainer, J. A. 2007. Quarterly Reviews of Biophysics, 40: 191–285. [Crossref], [PubMed], [Web of Science ®] , [Google Scholar]], which is now routinely used to rapidly determine ab initio low-resolution (>1 nm) protein structures [4 Hura, G. L. 2009. Nature Methods, 6: 606–614. [Crossref], [PubMed] , [Google Scholar]].     

Soft x‐ray techniques to study mesoscale magnetism

Femtosecond pulses from linac-based free-electron lasers are unique tools for future time-resolved experiments. In March 2004, BESSY published the Technical Design Report (TDR) for a free-electron-laser user facility that covers the VUV to soft X-ray range (BESSY FEL) [1 Krämer, D., Jaeschke, E. and Eberhardt, W., eds. 2004. Technical Design Report, Berlin, , Germany: BESSY.  [Google Scholar]]. This second-generation FEL facility is seeded and uses the High-Gain Harmonic-Generation (HGHG) [2 Doyuran, A. 2001. Phys. Rev. Lett., 86: 5902 [Google Scholar]] scheme to produce coherent radiation down to the 1 nm range.     

Lagrangian conditional moment closure model with flame group interaction for lifted turbulent spray jet flames

A new Lagrangian conditional moment closure (CMC) model is developed for multiple Lagrangian groups of sequentially evaporating fuel in turbulent spray combustion. Flame group interaction is taken into account as premixed combustion by the eddy breakup (EBU) model in terms of the probability of finding flame groups in the burned and the unburned state. Evaporation source terms are included in the two phase conditional transport equations, although they turn out to have negligible influence on the mean temperature field during combustion. The Lagrangian CMC model is implemented in OpenFOAM [1 H.G. Weller, G. Tabor, H. Jasak, and C. Fureby, A tensorial approach to computational continuum mechanics using object-oriented techniques, Comput. Phys. 12 (1998), pp. 620–631.[Crossref] [Google Scholar]] and validated for test cases in the Engine Combustion Network (ECN) [2 Engine Combustion Network. (2011). Available at http://www.sandia.gov/ecn. [Google Scholar],3 L.M. Pickett, C.L. Genzale, G. Bruneaux, L. Malbec, L. Hermant, C. Christian, and J. Schramm, Comparison of diesel spray combustion in different high-temperature, high-pressure facilities, SAE technical paper 2010-01-2106 (2010). [Google Scholar]]. Similar ignition delays and lift-off lengths are predicted by the incompletely stirred reactor (ISR) and the Eulerian CMC models due to relatively uniform conditional flame structure in the domain. The improved Lagrangian CMC model shows no abrupt reaction or oscillatory behaviour with an appropriate model constant K and gives results in better agreement with measurements lying between the predictions by ISR and Lagrangian CMC without flame group interaction.     

Ultrafast Soft X-ray Probing of Gas Phase Molecular Dynamics

The molecular ability to selectively and efficiently convert sunlight into other forms of energy like heat, bond change, or charge separation is truly remarkable. The decisive steps in these transformations often happen on a femtosecond timescale and require transitions among different electronic states that violate the Born-Oppenheimer approximation (BOA) [1 W. Domcke, D. Yarkony, and H. Köppel, Conical Intersections Electronic Structure, Dynamics &; Spectroscopy, World Scientific, Singapore (2004).[Crossref] , [Google Scholar]]. Non-BOA transitions pose challenges to both theory and experiment. From a theoretical point of view, excited state dynamics and nonadiabatic transitions both are difficult problems [2 F. Plasser, Theor. Chem. Acc. 131, 233902 (2012).[Crossref], [Web of Science ®] , [Google Scholar], 3 J. C. Tully, J. Chem. Phys. 137, 22A301 (2012).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]] (see Figure 1(a)). However, the theory on non-BOA dynamics has advanced significantly over the last two decades. Full dynamical simulations for molecules of the size of nucleobases have been possible for a couple of years [4 H. R. Hudock, J. Phys. Chem. A 111, 8500–8508 (2007).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar], 5 J. J. Szymczak, J. Phys. Chem. A 113, 12686–12693 (2009).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]] and allow predictions of experimental observables like photoelectron energy [6 S. Ullrich, Phys. Chem. Chem. Phys. 6, 2796 (2004).[Crossref], [Web of Science ®] , [Google Scholar]] or ion yield [7 H. Tao, J. Chem. Phys. 134, 244306 (2011).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]–9 M. Assmann, T. Weinacht, and S. Matsika, J. Chem. Phys. 144, 34301 (2016).[Crossref], [Web of Science ®] , [Google Scholar]]. The availability of these calculations for isolated molecules has spurred new experimental efforts to develop methods that are sufficiently different from all optical techniques. For determination of transient molecular structure, femtosecond X-ray diffraction [10 M. P. Minitti, Phys. Rev. Lett. 114, 255501 (2015).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar], 11 J. Küpper, Phys. Rev. Lett. 112, 083002 (2014). [Google Scholar]] and electron diffraction [12 J. Yang, Nat. Commun. 7, 11232 (2016).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]] have been implemented on optically excited molecules.     

The temperature-dependent electrical transport properties of liquid Sn using pseudopotential theory

We present the calculations of electrical resistivity, thermo-electric power and thermal conductivity based on the self-consistent approximation. The pseudopotential due to Hasegawa et al. [J. Non-Cryst. Solids 117/118, 300 (1990) M. Hasegawa, K. Hoshino, M. Watabe, and H. Young, J. Non-Cryst. Solids 117/118, 300 (1990).[Crossref], [Web of Science ®] , [Google Scholar]] for full electron–ion interaction, which is valid for all electrons and contains the repulsive delta function to achieve the necessary s-pseudisation, was used in the calculation. Temperature dependence of structure factor is achieved through temperature-dependent potential parameter in the pair-potential. The outcome of the present study is discussed in the light of other such results and with predictions of Wiedemann and Franz law up to moderately high temperature. Specially, high-temperature resistivity data necessitates the careful investigation of electron energy dispersion close to the Fermi level and possible metal to non-metal transition while going from dense-fluid to low density-fluid state. In the absence of experimental data at high temperature, these findings may serve as future guideline.     

Third User Workshop on High-Power Lasers at the Linac Coherent Light Source

On October 5–6, 2015, the third international user workshop focusing on high-power lasers at the Linac Coherent Light Source (LCLS) was held in Menlo Park, CA, USA [1 R. Falcone, S. Glenzer, and S. Hau-Riege, Synchrotron Radiation News 27(2), 56–58 (2014).[Taylor &; Francis Online] , [Google Scholar], 2 P. Heimann and S. Glenzer, Synchrotron Radiation News 28(3), 54–56 (2015).[Taylor &; Francis Online] , [Google Scholar]]. The workshop was co-organized by Los Alamos National Laboratory and SLAC National Accelerator Laboratory. More than 110 scientists attended from North America, Europe, and Asia to discuss high-energy-density (HED) science that is enabled by the unique combination of high-power lasers with the LCLS X-rays at the LCLS-Matter in Extreme Conditions (MEC) endstation.     

The mechanics and thermodynamics of edge fracture: the critical energy release rate,the compatibility constraint,and the bond potential

Following Gurtin and many others, the critical energy release rate is commonly identified as an ill-defined surface energy. The primary objectives of this paper are to clarify the definition of this surface energy and the role of the entropy inequality in the discussion of critical conditions. In view of an increasing emphasis on ab initio computations, a secondary objective is to show how the critical energy release rate and the compatibility constraint 1 Si, X, Oh, ES and Slattery, JC. 2010. Phil. Mag., 90: 655[Taylor & Francis Online] , [Google Scholar] can be used to solve a problem for which we have experimental data, using only ab initio estimates of surface tension and bond potential, both of which are increasingly available.     

Cryogenic Permanent Magnet Undulator Development at HZB/BESSY II

The costs of a synchrotron radiation facility scales approximately linearly with the length (FEL) or the circumference (storage ring) of the machine. It is always beneficial for the reduction in overall expenses to utilize short period in-vacuum undulators (IVUs) for X-ray production. This is the reason for the success of the IVU development which was started almost 20 years ago in Japan [1 T. Hara, J. Synch. Rad., 5, 403–405 (1998).[Crossref], [PubMed], [Web of Science ®] , [Google Scholar]–3 T. Tanaka, Proc. FEL Conf., Stanford, CA, 370–377 (2005). [Google Scholar]]. Today, IVUs are implemented into nearly all third-generation storage rings. Ten years ago, the concept of cryogenically cooled permanent magnet undulators (CPMUs) was proposed [4 T. Hara, Phys. Rev. ST Accel. Beams, 7, 050702-1-6 (2004).[Crossref] , [Google Scholar]]. The magnetic properties of rare earth magnets (i.e., the remanence and the coercivity) improve substantially at low temperatures. The remanence increases by about 15%, whereas the coercivity grows by a factor of three to four. Due to the performance gain and the low technical risk of CPMUs, such devices are under development all over the world. The first generation of CPMUs, with period lengths well below 20 mm, is successfully operated at ESRF [5 J. Chavanne, AIP Conf. Proc., SRI 2009, Melbourne, Australia 1234, 25–28 (2010). [Google Scholar], 6 J. Chavanne, Proc. PAC, Vancouver, BC, Canada, 2414–2416 (2009). [Google Scholar]], PSI [7 T. Tanaka et al, Phys. Rev. ST Accel. Beams, 12, 120702-1-5 (2009).[Crossref] , [Google Scholar]], DIAMOND [8 C. Ostenfeld and M. Pedersen, Proc. IPAC, Kyoto, Japan, 3093–3095 (2010). [Google Scholar]], SOLEIL [9 C. Benabderrahmane, J. Phys., Conf. Ser., SRI 2012, Lyon, France 425, 032019-1-4 (2013). [Google Scholar]], and SPring-8 [10 T. Tanaka, Private communication (2015). [Google Scholar]].