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DOE OSTI2024

Exploring the Tl 2H 2 potential energy surface: A comparative analysis with group 13 systems and experiment

Abstract Thallium chemistry is experiencing unprecedented importance. Therefore, it is valuable to characterize some of the simplest thallium compounds. Stationary points along the singlet and triplet TlH potential energy surface have been characterized. Stationary point geometries were optimized with the CCSD(T)/aug‐cc‐pwCVQZ‐PP method. Harmonic vibrational frequencies were computed at the same level of theory while anharmonic vibrational frequencies were computed at the CCSD(T)/aug‐cc‐pwCVTZ‐PP level of theory. Final energetics were obtained with the CCSDT(Q) method. Basis sets up to augmented quintuple‐zeta cardinality (aug‐cc‐pwCV5Z‐PP) were employed to obtain energetics in order to extrapolate to the complete basis set limits using the focal point approach. Zero‐point vibrational energy corrections were appended to the extrapolated energies in order to determine relative energies at 0 K. It was found that the planar dibridged isomer lies lowest in energy while the linear structure lies highest in energy. The results were compared to other group 13 MH (M = B, Al, Ga, In, and Tl) theoretical studies and some interesting variations are found. With respect to experiment, incompatibilities exist.

Chemistry↗

DOE OSTI2021

CeNTREX: a new search for time-reversal symmetry violation in the 205 Tl nucleus

The Cold molecule Nuclear Time-Reversal EXperiment (CeNTREX) is a new effort aiming for a significant increase in sensitivity over the best present upper bounds on the strength of hadronic time reversal (T) violating fundamental interactions. The experimental signature will be shifts in nuclear magnetic resonance frequencies of 205 Tl in electrically-polarized thallium fluoride (TlF) molecules. Here we describe the motivation for studying these T-violating interactions and for using TlF to do so. To achieve higher sensitivity than earlier searches for T-violation in TlF, CeNTREX uses a cryogenic molecular beam source, optical state preparation and detection, and modern methods of coherent quantum state manipulation. Details of the measurement scheme and the current state of the apparatus are presented, with quantitative measurements of the TlF beam. Lastly, the estimated sensitivity and methods to control systematic errors are discussed.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Nonperturbative phonon scatterings and the two-channel thermal transport in Tl 3 VSe 4

We review the role of nonperturbative phonon scattering in strongly anharmonic materials having ultralow lattice thermal conductivity with unusual temperature dependence. We take Tl 3 VSe 4 as an example and investigate its lattice dynamics using perturbation theory (PT) up to the fourth order and molecular dynamics (MD) with a machine-learning potential. We find distinct differences of phonon linewidth between PT and MD in the whole Brillouin zone. The comparison between the theoretical phonon linewidths and experiments suggests that PT severely underestimates the phonon scatterings, even when the fourth-order anharmonicity is included. Moreover, we extend our calculations to higher temperatures and evaluate the two-channel thermal conductivity based on the unified theory developed by Simoncelli et al. [Nat. Phys. 15, 809 (2019)]. We find a crucial coherence contribution to the total thermal conductivity at high temperatures. Our results pave the path for future studies of phonon properties and lattice thermal conductivities of strongly anharmonic crystals beyond the conventional PT realm.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Thermal Characterization of Tl 2 LiYCl 6 :Ce (TLYC)

Tl 2 LiYCl 6 :Ce (TLYC) is a new dual-detection elpasolite scintillator that can detect and distinguish between gamma rays and neutrons using pulse shape discrimination (PSD). It has a higher density and Z -number than the more mature and well-known elpasolite Cs 2 LiYCl 6 :Ce (CLYC), causing it to have a significantly better gamma-ray stopping power. These properties make TLYC an attractive alternative to CLYC for resource-constrained applications where size and weight are important, such as space or national security applications. Such applications may be subjected to a wide range of temperatures, and therefore, TLYC's performance was characterized for the first time over a temperature range of -20 °C to +50 °C in 10 °C increments. TLYC's thermal response effects on light-output linearity with energy, gamma-ray photopeak energy resolution, detected neutron energy, pulse shapes, and figure of merit (FOM) is analyzed and reported. The light output of TLYC was found to be linear with energy over the tested temperature range and was observed to decrease with increasing temperature. The decay time of the scintillation light output was observed to decrease with decreasing temperature at short times, leading to a decreasing PSD FOM. The gamma-ray photopeak energy resolution was also observed to degrade with decreasing temperature, due to an asymmetric broadening of the photopeak at low temperatures.

36 MATERIALS SCIENCE↗

NASA NTRS1986

Properties of a large NaI(Tl) spectrometer for the energy measurement of high-energy gamma rays on the Gamma Ray Observatory

A large NaI(Tl) spectrometer is expected to play a crucial role in the measurement of the energy spectra from an all-sky survey of high-energy celestial gamma rays on the Gamma Ray Observatory. The crystal size and requirements of space flight have resulted in a novel crystal-packaging and optics combination. The structure of this spectrometer and the operating characteristics determined in a test program using high energy positrons are described.

Hughes, E. B.↗

NASA NTRS1990

An explanation for the rise in T(sub c) in the Tl- and Bi-based high temperature superconductors

Using the plasmon exchange model for the high T(sub c) superconductor, it is shown that the T(sub c) rises with an increase in the number of CuO layers per unit cell, which is in agreement with recent observations in the Tl- and Bi-based compounds. The calculation also suggests that the sample will become superconducting in successive stages and that there is a saturation effect, i.e., that T(sub c) cannot be raised indefinitely by increasing the number of CuO layers.

Bose, S. M.↗

NASA NTRS1990

Novel superconducting phases of Tl-based compounds

Several new superconducting phases of the Tl-based compounds were prepared. Structural studies revealed cell lengths of 31.9 A and longer. Properties of Ce-containing compounds are also discussed.

Kostadinov, I. Z.↗

NASA NTRS1990

On the determination of iridium in diverse geological samples employing HPGe-coincidence/NaI(Tl)-anticoincidence spectrometry

This paper reports the Ir content of a variety of geological samples determined by the high-purity Ge-coincidence/NaI(Tl)-anticoincidence gamma-ray spectrometry (henceforth referred to as coincidence/anticoincidence technique) and by the conventional INAA. The advantages of this technique are: (1) the Ir content of the samples is obtained (ppm to a fraction of ppb ranges) not only by the 468.1 keV peak as in the conventional INAA but also by the 784.6 keV and 920.9 keV sum peaks, which gives more confidence in the values obtained; and (2) it is well suited for the samples with high Compton background for which it is difficult to measure the Ir content by the conventional INAA technique. The practical sensitivity of this technique depends on the sample matrix. Under present experimental conditions, it varied from 0.1 ng for Mn nodules and 0.004 ng for Libyan Desert Glass. Iridium values obtained on small (about 1 microg) olivine grains demonstrate the potential application of this new technique to microsamples. The principle and methodology of this new technique as well as its advantages and disadvantages over the conventional INAA are discussed.

Murali, A. V.↗

NASA NTRS1990

Enhanced ultrasonic attenuation of Tl-Ca-Ba-Cu-O at the superconducting transition

Temperature-dependent ultrasonic attenuation measurements have been performed on polycrystalline samples of Tl-Ca-Ba-Cu-O at various frequencies. An attenuation anomaly was observed close to the superconducting transition temperature T(c) (103 K) whose temperature position was frequency-independent. The attenuation decreased exponentially with temperature in the superconducting state for both transverse and longitudinal waves. It was also found that the temperature-dependent sound velocity showed a slope change around T(c).

Sun, K. J.↗

NASA NTRS1991

Development of high Tc (greater than 110K) Bi, Tl and Y-based materials as superconducting circuit elements

This report is presented in two parts. Part 1 deals primarily with Bi-based materials and a small amount of work on a Y-based composition while Part 2 covers work on Tl-based materials. In Part 1, a reliable and reproducible process for producing bulk bismuth-based superconductors has been developed. It is noted however, that a percentage of the tapecast material experiences curling and fracturing after a 30 hour sintering period and is thus in need of further examination. The Bi-Sr-Ca-Cu-O (BSCCO) material has been characterized by critical temperature data, X-ray diffraction data, and surface morphology. In the case of T sub c, it is not critical to anneal the material. It appears that the BSCCO material has the possibility of producing a better grounding strap than that of the 123 material. Attempts to reproduce near room temperature superconductors in the Y-Ba-Cu-O system were unsuccessful. In Part 2, several methods of processing the high temperature superconductor Tl2Ba2Ca2Cu3O10 were investigated; i.e., different precursor compositions were sintered at various sintering times and temperatures. The highest superconductig temperature was found to be 117.8K when fired at 900 C for three hours. Higher sintering temperatures produced a melted sample which was nonsuperconducting at liquid nitrogen temperature. Also, a preliminary study found Li2O substitutions for copper appeared to increase the transition temperature and create fluxing action upon sintering. It was suggested that lower sintering temperatures might be obtained with lithium additions to produce reliable Tl2Ba2Ca2Cu3O10 processing methods.

Haertling, Gene H.↗

NASA NTRS1991

Synthesis and superconducting properties of Tl-Ba-Ca-Cu-O films

Tl-Ba-Ca-Cu-O superconducting films were synthesized by sputtering either from a single target or from two oxide targets in a symmetric configuration. Films with zero resistance Tc of up to 122 K were obtained after various postannealing treatments at 870-950 C under an oxygen atmosphere. The composition of the films is not very homogeneous on the submicrometer scale. The critical current of these films at 77 K is in the 1000 A/sq cm to 10,000 A/sq cm range, which is much smaller than that of films prepared on SrTiO3 and LaAlO3 substrates. The low critical current density in these films is probably due to the granularity in the films. The morphology, structure, and magnetic and superconducting properties of the films were studied. Films prepared by two different sputtering techniques have similar results which depend mostly on the film compositions and their annealing conditions. It is found that the induced magnetic flux in the film decreases rapidly with increasing temperature, indicating weak flux pinning.

Liou, S. H.↗

NASA NTRS1990

Pulsed laser deposition of Tl-Ca-Ba-Cu-O films

Pulsed laser deposition is a technique commonly used to deposit high quality thin films of high temperature superconductors. This paper discusses the results obtained when this technique is applied to the deposition of Tl-Ca-Ba-Cu-O thin films using a frequency doubled Nd:YAG laser operating at 532 nm and an excimer laser operating at 248 nm. Films with onset temperatures of 125 K and zero resistance temperatures of 110 K deposited on (100) oriented MgO from a composite Tl2Ca2Ba2Cu3Ox target were obtained at both wavelengths upon appropriate post deposition annealing. Films deposited at 532 nm exhibit a rough surface, while those deposited at 248 nm are smooth and homogeneous. Upon annealing, films deposited at both wavelengths are single phase Tl2Ca2Ba2Cu3Ox.

Ianno, N. J.↗

NASA NTRS1991

Development of high Tc (greater than 110K) Bi, Tl and Y-based materials as superconducting circuit elements

Experimental work was continued on the development and characterization of bulk and hot pressed powders and tapecast materials in the Bi-Sr-Ca-Cu-O and Tl-Ba-Ca-Cu-O systems. A process for producing warp-free, sintered, superconducting tapes of Bi composition Bi1Sr2Ca2 Cu3O(x) was established. The procedure requires a triple calcination at 830 C for 24 hours and sintering at 845 C from 20 to 200 hours. Hot pressing the triple calcined powder at 845 C for 6 hours at 5000 psi yielded a dense material, which on further heat treatment at 845 C for 24 hours, exhibited a Tc of 108.2K. The Bi compositions were found to be much less oxygen sensitive than the Y compositions. This was especially noted in the case of the hot pressed materials which were superconducting as hot pressed, a condition that could not be achieved in the Y compositions. Safire-type grounding links are in the process of being fabricated from these materials.

Haertling, Gene↗

NASA NTRS1991

An explanation for the rise in Tc in the Tl- and Bi-based high temperature superconductors

Bose, S. M.↗

NASA NTRS1992

Conductor-backed coplanar waveguide resonators of Y-Ba-Cu-O and Tl-Ba-Ca-Cu-O on LaAlO3

Conductor-backed coplanar waveguide (CBCPW) resonators operating at 10.8 GHz have been fabricated from Tl-Ba-Ca-O (TBCCO) and Y-Ba-Cu-O (YBCO) thin films on LaAlO3. The resonators consist of a coplanar waveguide (CPW) patterned on the superconducting film side of the LaAlO3 substrate with a gold ground plane coated on the opposite side. These resonators were tested in the temperature range from 14 to 106 K. At 77 K, the best of our TBCCO and YBCO resonators have an unloaded quality factor (Qo) 7 and 4 times, respectively, larger than that of a similar all-gold resonator. In this study, the Qo's of the TBCCO resonators were larger than those of their YBCO counterparts throughout the aforementioned temperature range.

Miranda, F. A.↗

NASA NTRS1993

Development of high Tc (greater than 100 K) Bi, Tl and Y-based materials as superconducting circuit elements

Results on this project over the past three years have shown that the Bi and Tl-based superconducting materials in bulk form are noticeably different from the Y-based 123 material in that superconductivity is considerably harder to achieve, maintain and reproduce. This is due primarily to the difficulty in obtaining the higher Tc phase in pure form since it commonly co-exists with other undesirable, lower Tc phases. In particular, it has been found that long processing times for calcining and firing (20 - 200 hrs.) and close control of temperatures which are very near the melting point are required in order to obtain higher proportions of the desirable, high Tc (2223) phase.

Haertling, Gene↗

NASA NTRS1993

Sensitivity of LDEF foil analyses using ultra-low background germanium vs. large NaI(Tl) multidimensional spectrometers

Cobalt foils and stainless steel samples were analyzed for induced Co-60 activity with both an ultra-low background germanium gamma-ray spectrometer and with a large NaI(Tl) multidimensional spectrometer, both of which use electronic anticoincidence shielding to reduce background counts resulting from cosmic rays. Aluminum samples were analyzed for Na-22. The results, in addition to the relative sensitivities and precisions afforded by the two methods, are presented.

Reeves, James H.↗

NASA NTRS1993

Low temperature phase formation of Tl-based superconducting thin films in reduced oxygen atmosphere

Tl-Ba-Cu-Cu-O superconducting thin films were prepared by magnetron sputtering with postannealing in a reduced oxygen atmosphere. Single-phase Tl2Ba2Ca2Cu3O(x) can form on the MgO substrate at 800 C under P(O2) about 0.1 atm. However the phase formation temperature can be affected by the starting composition of the film. Tl1Ba2Ca2Cu3O(x) phase can be formed by simply lowering the Tl2O pressure. The thermal stability of Tl1Ba2Ca2Cu3O(x) phase was studied by resistivity measurements at high temperatures.

Wu, C. Y.↗