Uranium Sites Research Articles

Estimation of natural radioactivity in the soil samples around the uranium site, royal village, Khandela, Sikar district, Rajasthan.

The measurements of activity concentration of radium ( 226Ra ), thorium ( 232Th) and potassium ( 40K ) natural radionuclides using high purity germanium ( HPGe ) detector to assess harmful effects on people residing around Royal Uranium Site, Sikar, Rajasthan, India. The activity concentrations range from 29.03±3.72 to 69.95±4.07Bq/kg for 226Ra with a mean value of 47.01Bq/kg, 57.99±6.13 to 113.94±6.54Bq/kg with a mean value of 86.56Bq/kg for 232Th,678.19±76.36 to 1426.55±81.32Bq/kg for 40K with a mean value of 1195Bq/kg. Average Radium Equivalent Activity was measured 261.59±35.48Bq/kg. The total outdoor absorbed gamma dose rate ranged from 78.42 to 157.91 nGy/h with a mean value of 122.12 nGy/h.The average annual effective dose equivalent outdoors and indoors was found 0.75mSv.Mean external (Hex) and internal (Hin) hazard indices are measured 0.70 and 0.82, respectively, for the study area.

Pressure-induced evolution of the lattice dynamics for selected UO3 polymorphs

Uranium trioxide (UO3) is a stable chemical form of uranium oxide with multiple polymorphs found throughout the nuclear fuel cycle. The pressure-induced changes in the structure and lattice dynamics of four of these polymorphs are simulated with density functional perturbation theory and analyzed. Two phases, α- and δ-UO3 are found to exhibit an isotropic response to pressure and do not undergo any changes in coordination geometry up to ∼40 GPa. In contrast, the other two phases investigated, β- and γ-UO3, exhibit an anisotropic response to pressure. Decomposition of the phonon eigenvectors allows us to assign specific pressure-induced structural changes to individual phonon modes. This analysis has been performed on a per atom basis for the relatively simple α- and δ-UO3 structures, which have one symmetrically unique uranium site, and on a per coordination environment basis for β- and γ-UO3, which have multiple U sites.

Ferromagnetic Crossover within the Ferromagnetic Order of U7Te12

We investigate the physical properties of a single crystal of uranium telluride U$_{7}$Te$_{12}$. We have confirmed that U$_{7}$Te$_{12}$ crystallizes in the hexagonal structure with three nonequivalent crystallographic uranium sites. The paramagnetic moments are estimated to be approximately 1 $\mu_{\rm B}$ per the uranium site, assuming a uniform moment on all the sites. A ferromagnetic phase transition occurs at $T_{\rm C}=48$ K, where the in-plane magnetization increases sharply, whereas the out-of-plane component does not increase significantly. With decreasing temperature further below $T_{\rm C}$ under field-cooling conditions, the out-of-plane component increases rapidly around $T^{\star}=26$ K. In contrast, the in-plane component hardly changes at $T^{\star}$. Specific heat measurement indicates no $\lambda$-type anomaly around $T^{\star}$, so this is a cross-over suggesting a reorientation of the ordering moments or successive magnetic ordering on the part of the multiple uranium sites.

Density functional theory investigations into the magnetic ordering of U3O8

Density functional theory (DFT) has been highly successful in supporting experimental materials science; however, a correct electronic ground state is required to realize the full theoretical capacity of DFT. The uranium oxides, $\ensuremath{\alpha}\ensuremath{-}{\mathrm{U}}_{3}{\mathrm{O}}_{8}$ in particular, are simultaneously technologically important materials and theoretically challenging for DFT because the uranium magnetic ground state is not obvious. This is true for both experiment and theory---magnetic susceptibility measurements indicate an antiferromagnetic (AFM) ground state with transitions near 4.2 and 8.0 K, but the ordering itself is not known. Theoretical literature reports are in contradiction, with independent studies finding paramagnetic, ferromagnetic (FM), and AFM states as the lowest energy configuration. However, recent inelastic neutron scattering experiments suggested an uninvestigated magnetic structure with ordering along the [0.5 1 1] plane, motivating a theoretical reinvestigation. Using this insight, we calculated the relative energy of FM and AFM orderings along [0.5 1 1], [0.5 0 0], [0 1 0], and [0 0 1] using noncollinear DFT calculations with spin-orbital coupling. We found that the [0.5 1 1] AFM structure is lower in energy than FM or AFM orderings along the low Miller index directions. We also investigated polarization of the magnetic moment along each lattice vector and found that polarization along the out-of-plane direction is the energetically preferred orientation for the AFM structures. Additionally, we found in all calculations that moments initially pointing along the in-plane lattice vectors significantly relax until they point along the coordinate between the two crystallographically distinct uranium sites with complex noncollinear magnetic configurations. The new [0.5 1 1] AFM magnetic structure provides an additional path forward toward understanding the electronic structure of \ensuremath{\alpha}-${\mathrm{U}}_{3}{\mathrm{O}}_{8}$ and lends theoretical credibility to recent neutron scattering results.

Geological risk management process and its particularities for a uranium site - case study

Anthropogenic radioactive pollution of the environment resulting from the research and exploitation of uranium resources is a topical issue for the scientific community because it represents a threat to people’s health conditions and has a highly negative impact on the environment. The sources of radioactive pollution are due to the presence of low-level radioactive tailings and poor ore dumps resulting from the exploration and exploitation of uranium ore deposits. Uranium under the action of environmental factors can reach the groundwater, the river network, and the food chain, respectively. The contaminated food and water may cause diseases and even cancer. An important role in the pollution spreading is played by geological phenomena, the most important being landslides. Thus arises the need for geological risk management. The present study aims to implement a geological risk management system through methods of assessment, monitoring, and prediction of geological risk for a chosen uranium site. The waste rock and water samples analysis pointed out the radioactive contamination risk. The simulated scenarios in the area exposed to subsidence phenomena showed the activity of increasing the concentration of radioactive waste in the hydrographic system’s groundwater in the studied site, in a time interval of 4120 days (11.29 years): it rapidly increased in the first 1000 days (from 0.0 to 0.0033), after which it decreased in intensity until day 2500 (from 0.0033 to 0.0048), and it is supposed to stagnate after day 2500 until day 4120 when the simulation ended. The results emphasised the radioactive contamination spreading risk in the case when the subsidence phenomenon takes place.

An Investigation on Structural Properties of Radiation Damaged ZrSiO4 Using X-Ray Diffractometry and DFT

Naturally occurring Zirconium minerals contain interstitial impurities of radioactive elements. Over a period of time due to alpha decay, the structure of minerals degrades through an internal bombardment process called metamictization. These metamict minerals proposed to be used as reference signatures for Naturally Occurring Radioactive Materials (NORM) Monitoring because of their unique parameters in structural properties. We have investigated structural damage of partially metamict Zirconium Silicate samples (ZrSiO4), collected from Lambapur - Peddagattu region, Andhra Pradesh, India known for larger Uranium deposits. X-Ray Diffractometry data was used to study structural parameters experimentally. Structural properties of ZrSiO4 belonging to space group I41/amd have been modeled and studied theoretically using Quantum ATK within local density approximation and generalized gradient approximation in-order to compare the structural properties obtained from the experimental data. We have investigated that the lattice parameters increased with a = 0.033 Å and c = 0.051 Å in the sample collected from proposed Uranium sites. We propose to use the lattice parameter variability of ZrSiO4 as a tracer tool in nuclear forensics.

Feasibility of ZrSiO4 as reference signature in naturally-occurring radioactive elements for the application of radioactivity monitoring

Radioactivity monitoring post-cold war has become more complex due to the nuclear fallout and the surge in use of radioactive materials. This requires novel methods to detect, trace and distinguish natural and anthropogenic radioactive sources in the environment. We explored the feasibility of using ZrSiO4 (Zircon), as a reference signature for radioactivity monitoring due to the unique phenomenon of metamictization. We investigated the variations in microstructural properties of Zircon samples collected from a proposed Uranium site to identify these signatures using analytical techniques such as Gamma-ray Spectroscopy, XRD and Raman spectrum analysis. Besides elevated levels of radioactivity, the samples exhibited distinct properties such as increased lattice parameters observed from the XRD analysis and dramatic broadening of A1g (439 cm−1) and B1g (1008 cm−1) vibrational modes in the Raman spectrum. Structural parameters were further analyzed by modeling the crystal from experimentally observed lattice parameters. Ab-initio calculations were then performed on the modeled structure providing more insight into the microstructural variations. Samples collected from proposed Uranium mines indicate an increase of 1.226% and 0.9389% in Si–O and Zr–O bond lengths of the Zircon crystal signifying the ongoing process of metamictization from radiation damage. By correlating radioactivity levels with the lattice parameters variations of the collected samples, the study establishes a linear relation between the degree of damage to a mineral's crystal structure and the amount of radioactivity. We propose to use the variations in damage found in a mineral's structure as a nuclear forensic signature for advanced assessment of accumulated radioactivity in a particular geographical location.

Bioleaching of Uranium Tailings as Secondary Sources for Rare Earth Elements Production

Tailings from inactive uranium mine sites represent a potential secondary source of rare earth elements (REEs). For this study, two mine tailings (DT and RAT) from restored uranium sites in Ontario, Canada, were used. Bioleaching experiments were conducted with a mix of native sulfur- and iron-oxidizing bacteria to test the solubilization of REEs, U and Th at different temperatures (20, 30 and 40 °C). The selective recovery of REEs from bioleaching solution was evaluated using different ion exchange resins. The mineralogical characterization revealed that DT tailings were mainly composed of quartz, pyrite, gypsum and silicates, whereas RAT tailings were mainly composed of quartz. The maximum solubilization of heavy and light REEs (HREEs and LREEs, respectively), Th and U reached 54%, 6%, 60% and 51% for RAT after 35 days at pH 2, T = 30 °C and pulp density = 10% (w/v). Higher extraction yields were obtained for DT, with 58% of HREEs, 14% of LREEs, 85% of Th and 89% of U solubilized under the same conditions. The use of Lewatit TP272 resin for the recovery of Sc (94%) and U (99%) followed by the Lewatit SP112 resin for the recovery of Th (57%) and REEs (81% LREEs and 65% HREEs) seemed a promising method for the co-extraction of the key elements from the bioleaching solution.

Landslide-Induced Mass Transport of Radionuclides along Transboundary Mailuu-Suu River Networks in Central Asia

Seismically triggered landslides are a major hazard and have caused severe secondary losses. This problem is especially important in the seismic prone Mailuu-Suu catchment in Kyrgyzstan, as it hosts disproportionately sensitive active or legacy uranium sites with deposited radioactive extractive wastes. These sites show a quasi-continuous release of radioactive contamination into surface waters, and especially after natural hazards, a sudden and massive input of pollutants into the surface waters is expected. However, landslides of contaminated sediments into surface waters represent a substantial exposure pathway that has not been properly addressed in the existing river basin management to date. To fill this gap, satellite imagery was massively employed to extract topography and geometric information, and the seismic Scoops3D and the one-dimensional numerical model, Hydrologic Engineering Centre, River Analysis System (HEC-RAS), were chosen to simulate the landslide-induced mass transport of total suspended solids (TSS) and natural radionuclides (Pb-210 as a proxy for modeling purposes) within the Mailuu-Suu river networks under two earthquake and two hydrological scenarios. The results show that the seismically vulnerable areas dominated in the upstream areas, and the mass of landslides increased dramatically with the increase of earthquake levels. After the landslides, the concentrations of radionuclides increased suddenly and dramatically. The peak values decreased along the longitudinal gradient of river networks, with the concentration curves becoming flat and wide in the downstream sections, and the transport speed of radionuclides decreased along the river networks. The conclusions of this study are that landslides commonly release a significant amount of pollutants with a relatively fast transport along river networks. Improved quantitative understanding of waterborne pollution dispersion across national borders will contribute to better co-ordination between governments and regulatory authorities of riparian states and, consequently, to future prevention of transnational political conflicts that have flared up in the last two decades over alleged pollution of transboundary water bodies.

Mapping the Alteration Zones for Uranium Exploration in Gabal Abu Garadi Area Central Eastern Desert, Egypt, Using Aster Data

The integration of the ASTER image processing and the airborne spectrometric Gamma-Ray interpretation helped in identifying the types and illustrating the distributions of the probable sites for radioactive mineralization at the Gabal Abu Garadi area. Appling various techniques of image processing for Landsat OLI and ASTER satellite to discrimination the differently exposed rock units and extract major and minor structural lineaments. This study resulted that the ASTER VNIR-SWIR bands are effectively used for clarifying the sericite, kaolinite, chlorite, illite and hematite bearing alteration zones, whereas the ASTER TIR bands are most effective in delineation of the silica-rich zones which could be pathfinders for radioactive mineralization within the study area. The resultant alteration maps show good coincidence with the explored uranium sites and suggest further similar unexplored sites. The predominance of low eTh/eU= 1.31 indicates U mobilization and reveals that magmatic differentiation was not the sole process responsible for the concentration of these radioactive elements in the Abu Gradi area. Where the presence of adequate structures such as shear zones and fault planes facilitates the circulation of hydrothermal fluids and meteoric waters leading to mobilization and a redistribution of uranium. This paper could assist the principals of uranium exploration techniques.

Structural features of solid-solid phase transitions and lattice dynamics in U3O8

Triuranium octoxide $({\mathrm{U}}_{3}{\mathrm{O}}_{8})$ undergoes an orthorhombic to hexagonal structural phase transition near ${T}_{s}=305{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$, and a separate nonstructural phase transition at ${T}_{c}=210{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$. The later transition has previously been associated with temperature-induced fluctuations in the uranium oxidation state. A discontinuity in the slope of electrical conductivity versus temperature measurement at $210{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$ has supported this idea. The orthorhombic phase has three crystallographic sites in two distinct oxidation configurations [2 U(V) and 1 U(VI)], whereas the hexagonal phase has one distinct uranium site. High-resolution x-ray diffraction measurements eliminate the possibility of superlattice Bragg reflections to less than 0.2 ${\mathrm{e}}^{\ensuremath{-}}$ scattering power and ${\mathrm{U}}_{3}{\mathrm{O}}_{8}$ is not metallic; consequently, the presence of oxidation fluctuations is required for charge balancing. Interestingly, the order-to-disorder transition occurs at a much lower temperature than the structural transition. Using temperature-dependent x-ray diffraction and Raman spectroscopy, we show anisotropic lattice expansion in the in-plane $b$ and $c$ lattice constants. A specific discontinuity in the temperature derivatives of the $b$ and $c$ lattice constants are the first reported structural signatures of the order-to-disorder transition, suggestive of a change in local U--O coordination. Phonon frequencies of ${\mathrm{U}}_{3}{\mathrm{O}}_{8}$ measured by Raman spectroscopy show significant temperature-dependent dynamics. Redshifting of several modes between 40 and $300{\phantom{\rule{0.16em}{0ex}}}^{\ensuremath{\circ}}\mathrm{C}$ cannot be explained by unit cell expansion alone because the unit cell volume decreases in this region. Instead, we show that phonon frequencies are highly correlated with the anisotropic lattice expansion/contraction along specific crystallographic directions.

Pilot Test of the Permeable Reactive Barrier for Removing Uranium from the Flooded Gunnar Pit

This work reports on applying iron oxide coated sand (IOCS) media in an experimental permeable reactive barrier to remove uranium (U) species from uranium containing water. A field study was conducted at the legacy Gunnar uranium mine & mill site that was abandoned in the 1960s with limited to no decommissioning. The flooded Gunnar mine pit presently contains about 3.2 million m3 of water contaminated by dissolved U (1.2 mg/L), Ra-226 (0.4 Bq/L), and minor concentrations of other contaminants (As, Se, etc.). The water is seeping over the pit rim into Lake Athabasca, posing potential environmental and health concerns. IOCS media can be used to immobilize uranium species through an adsorption process. Herein, the preparation of hydrous ferric oxide sorbents and their supported forms onto silica sands is described. Fourier transform infrared spectroscopy (FTIR) and powder X-ray diffraction (pXRD) were used for structural characterization. The adsorption properties of the IOCS sorbent media were modeled by the Langmuir adsorption isotherm, where a maximum uranium uptake capacity was estimated. Bench-scale adsorption kinetic experiments were also performed before moving to a field trial. Based on these lab results and input on field-scale parameters, a pilot permeable reactive barrier was fabricated and a field test conducted near the Gunnar pit in June 2019. This pilot test provided technical data and information needed for designing a full-scale permeable barrier that employs the IOCS media. This approach can be applied for in-situ water treatment at Gunnar and other legacy uranium sites.

Distribution of organically bound tritium (OBT) activity concentrations in aquatic biota from eastern Canada

A survey of eastern Canadian biota was conducted to determine the distribution of activity concentrations of organically bound tritium (OBT). Fish samples were collected from Lake Ontario and the St. Lawrence River in areas continuously receiving inputs of tritiated water (HTO) from operating nuclear power plants, and from Lake Nipissing, a background area. Components of their aquatic environments were sampled. The data collected also provides some insight on how tritium activity concentrations in ambient water influence tissue free water tritium (TFWT) and OBT activity concentrations in biological tissues.Using an ALOKA liquid scintillation system, fish TFWT and OBT were quantified. Fish TFWT averaged 1.6 ± 0.1 Bq/L in Lake Nipissing and 3.1 ± 0.3 Bq/L in Lake Ontario. In contrast, TFWT ranged from 11.1 to 80.8 Bq/L in the St. Lawrence River near the Gentilly-2 Canada Deuterium Uranium (CANDU) site. Fish tissue OBT levels were 4.0 ± 0.4 Bq/L and 5.3 ± 0.2 Bq/L for Lake Nipissing and Lake Ontario, respectively, and between 18.1 and 134.2 Bq/L for CANDU sites.The activity concentrations of TFWT and OBT were reviewed for algae, freshwater mussel and various fish samples collected near Gentilly-2, Pickering and Darlington Nuclear Power Generating Stations. TFWT in aquatic biota was found to correlate with the tritium activity concentrations measured in waters at the time of sampling (TFWT/HTO of ambient water was 0.3–4.3). The OBT concentration factors (OBT/HTO of ambient water) were found to be higher in freshwater mussels (between 17 and 47) compared to algae and fish (0.3–10). These results point to a heterogeneous distribution of biota OBT content in these aquatic ecosystems. It was also noted that all fish and algae samples were found to be within the range of tritium activity concentrations that has been historically measured in the same waters. Values in freshwater mussels were above this range.

Geophysical inversion contributions to mineral exploration: lessons from the Footprints project

Magnetic and gravity inversions are used to create 2D or 3D models of the magnetic susceptibility and density, respectively, using potential field data. Unconstrained inversions generate an output based on mathematical constraints imposed by the inversion algorithm. Constrained inversions integrate lithological, structural, and petrophysical information in the inversion process to produce more geologically meaningful results. This study analyses the validity of this assertion in the context of the NSERC-CMIC Mineral Exploration Footprints project. Unconstrained and constrained geophysical inversions were computed for three mining sites: a gold site (Canadian Malartic, Québec), a copper site (Highland Valley, British Columbia), and a uranium site (Millennium – McArthur River, Saskatchewan). After initially computing unconstrained inversions, constrained inversions were developed using physical property measurements, which directly link geophysics to geology, and lithological boundaries extracted from an interpreted geological model. While each derived geological model is consistent with the geophysical data, each site exhibited some magnetic complexity that confounded the inversion. The gold site includes regions with a strong magnetic signature that masks the more weakly magnetic zone, thereby hiding the magnetic signature associated with the ore body. Initial unconstrained inversions for the copper site yielded solutions with invalid depth extent. A consistency between the constrained model and the geological model is reached with iterative changes to the depth extent of the model. At the uranium site, the observed magnetic signal is weak, but the inversion provided some insights that could be interpreted in terms of an already known complexly folded geological model.

210Po sequential extraction applied to wetland soils at uranium mining sites

Former uranium mining activities have led to the presence of naturally occurring nuclides embedded in soil. Such activities have also modified the secular equilibrium between radionuclides in 238U decay series. The objective of this paper is to quantify the long-term effect of former uranium mining activities on the behavior of the final radionuclide in the 238U-series, i.e. polonium-210 (210Po), present in soils. Soil samples are extracted from two uranium sites in France, specifically a quarried site and a natural site. The polonium distribution is studied within the various soil fractions, namely: water soluble, exchangeable, bound to carbonates, bound to iron/manganese oxides, bound to organic matter, and residual. 210Po is mainly found in the residual fraction of both study sites (87–90%), followed by the carbonates fraction (5–9%). The 210Po activity in the other fractions is very small in comparison with total activity.

Phase transition and compressibility study of UOs2 under pressure

High-pressure X-ray diffraction studies on MgCu2 type phase of UOs2 have been carried out up to 36 GPa. The compound remains in its parent phase up to 12 GPa with bulk modulus 261 GPa. Beyond 12 GPa, a first order phase transformation is observed. The phase transition is sluggish in nature and completes at 20.1 GPa. The high-pressure phase is found to be a hexagonal cell with lattice parameters a = 3.013 Å and c = 4.267 Å. Charge density calculations show that uranium tetrahedra in the lattice are responsible for the phase transition. The density of state plots at Fermi level, wherein a pseudogap originates at high pressures, confirms the existence of a high pressure phase and uranium site is found to contribute significantly to such changes in density of state. The retrievable high pressure phase is found to be the least compressible among uranium intermetallic compounds with bulk modulus of 366 GPa.

Structural features of uranium-protein complexes

Uranium toxicity depends on its chemical properties rather than on its radioactivity and involves its interaction with macromolecules. Here, a systematic survey of the structural features of the uranyl sites observed in protein crystal structures deposited in the Protein Data Bank is reported. Beside the two uranyl oxygens, which occupy the axial positions, uranium tends to be coordinated by five other oxygen atoms, which occupy the equatorial vertices of a pentagonal bipyramid. Even if one or more of these equatorial positions are sometime empty, they can be occupied only by oxygen atoms that belong to the carboxylate groups of Glu and Asp side-chains, usually acting as monodentate ligands, to water molecules, or to acetate anions. Although several uranium sites appear undefined or unrefined, with a single uranium atom that lacks the two uranyl oxygen atoms, this problem seems to become less frequent in recent years. However, it is clear that the crystallographic refinements of the uranyl sites are not always well restrained and a better parametrization of these restraints seems to be necessary.

Electronic and Magnetic Structures, Magnetic Hyperfine Fields and Electric Field Gradients in UX3 (X = In, Tl, Pb) Intermetallic Compounds

Cubic uranium compounds such as UX3 (X is a non-transition element of groups IIIA or IVA) exhibit highly diverse magnetic properties, including Pauli paramagnetism, spin fluctuation and anti-ferromagnetism. In the present paper, we explore the structural, electronic and magnetic properties as well as the hyperfine fields (HFFs) and electric field gradients (EFGs) with quadrupole coupling constant of UX3 (X = In, Tl, Pb) compounds using local density approximation, Perdew–Burke–Ernzerhof parametrization of generalized gradient approximation (PBE-GGA) including the Hubbard U parameter (GGA + U), a revised version of PBE-GGA that improves equilibrium properties of densely packed solids and their surfaces (PBEsol-GGA), and a hybrid functional (HF-PBEsol). The spin orbit-coupling calculations have been added to investigate the relativistic effect of electrons in these materials. The comparison between the experimental parameters and our calculated structural parameters we confirm the consistency and effectiveness of our theoretical tools. The computed magnetic moments show that magnetic moment increases from indium to lead in the UX3 family, and all these compounds are antiferromagnetic in nature. The EFGs and HFFs, as well as the quadrupole coupling constant of UX3 (X = In, Tl, Pb), are discussed in detail. These properties primarily originate from f and p states of uranium and post-transition sites.

Electronic and magnetic properties of the ferromagnetic superconductor UCoGe

The electronic structure and x-ray magnetic circular dichroism (XMCD) spectra of the ferromagnetic superconductor UCoGe at the U N4,5, Ge and Co K and Co L2,3 edges were investigated theoretically from first principles, using the fully relativistic Dirac linear muffin-tin orbital band structure method. The electronic structure is obtained with the local spin-density approximation (LSDA), as well as with a generalization of the LSDA+U method which takes into account the non-diagonal occupation matrix (in spin indexes) of localized electrons. A stable ferromagnetic ground state was found. The uranium total magnetic moment is quite small (about −0.171μB) in the LSDA approximation as a result of almost complete cancellation between the spin magnetic moment of 0.657 μB and the opposite orbital magnetic moment of −0.828 μB, resulting from strong spin-orbit coupling at the uranium site. Valency of U ion in UCoGe is close to 3+. The ratio orbital and spin magnetic moments Ml/Ms ranged from 1.163 in the GGA approa...

Raman active high energy excitations in URu2Si2

We have performed Raman scattering measurements on URu2Si2 single crystals on a large energy range up to ∼1300cm−1 and in all the Raman active symmetries as a function of temperature down to 15K. A large excitation, active only in the Eg symmetry, is reported. It has been assigned to a crystal electric field excitation on the Uranium site. We discuss how this constrains the crystal electric field scheme of the Uranium ions. Furthermore, three excitations in the A1g symmetry are observed. They have been associated to double Raman phonon processes consistently with ab initio calculations of the phonons dispersion.