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Weak Electron Phonon Coupling and Deep Level Impurity for High Thermoelectric Performance Pb 1–x Ga x Te
High ZT of 1.34 at 766 K and a record high average ZT above 1 in the temperature range of 300-864 K are attained in n-type PbTe by engineering the temperature-dependent carrier concentration and weakening electron–phonon coupling upon Ga doping. The experimental studies and first principles band structure calculations show that doping with Ga introduces a shallow level impurity contributing extrinsic carriers and imparts a deeper impurity level that ionizes at higher temperatures. This adjusts the carrier concentration closer to the temperature-dependent optimum and thus maximizes the power factor in a wide temperature range. The maximum power factor of 35 μW cm -1 K -2 is achieved for the Pb 0.98 Ga 0.02 Te compound, and is maintained over 20 μWcm-1 K-2 from 300 to 767 K. Band structure calculations and X-ray photoelectron spectroscopy corroborate the amphoteric role of Ga in PbTe as the origin of shallow and deep levels. Additionally, Ga doping weakens the electron–phonon coupling, leading to high carrier mobilities in excess of 1200 cm 2 V -1 s -1 . Enhanced point defect phonon scattering yields a reduced lattice thermal conductivity. Here, we provide a new avenue, beyond the conventional shallow level doping, for further improving the average ZT in thermoelectric materials.
Development of a Low-Level Ar-37 Calibration Standard
Argon-37 is an important environmental signature of an underground nuclear explosion. Producing and quantifying low-level 37Ar standards is an important step in the development of sensitive field measurement instruments for use during an On-Site Inspection, a key provision of the Comprehensive Nuclear-Test-Ban Treaty. This paper describes progress at Pacific Northwest National Laboratory (PNNL) in the development of a process to generate and quantify low-level 37Ar standard material, which can then be used to calibrate sensitive field systems at activities consistent with soil background levels. The 37Ar used for our work was generated using a laboratory-scale, high-energy neutron source to irradiate powdered samples of calcium carbonate. Small aliquots of 37Ar were then extracted from the head space of the irradiated samples. The specific activity of the head space samples, mixed with P10 (90% stable argon:10% methane by mole fraction) count gas, is then derived using the accepted Length-Compensated Internal-Source Proportional Counting method. Due to the low activity of the samples, a set of three Ultra-Low Background Proportional-Counters designed and fabricated at PNNL from radio-pure electroformed copper was used to make the measurements in PNNL’s shallow underground counting laboratory. Very low background levels (<10 counts/day) have been observed in the spectral region near the 37Ar emission feature at 2.8 keV. Two separate samples from the same irradiation were measured. The first sample was counted for 12 days beginning 28 days after irradiation, the second sample was counted for 24 days beginning 70 days after irradiation (the half-life of 37Ar is 35.0 days). Both sets of measurements were analyzed and yielded very similar results for the starting activity (~0.1 Bq) and activity concentration (0.15 mBq/ccSTP argon) after P10 count gas was added. A detailed uncertainty model was developed based on the ISO Guide to the Expression of Uncertainty in Measurement. This paper presents a discussion of the measurement analysis, along with assumptions and uncertainty estimates.
Atomic-level heterogeneity and defect dynamics in concentrated solid-solution alloys
Performance enhancement of structural materials in extreme radiation environments has been activelyinvestigated for many decades. Traditional alloys, such as steel, brass and aluminum alloys, normallycontain one or two principal element(s) with a low concentration of other elements. While these existin either a mixture of metallic phases (multiple phases) or in a solid solution (single phase), limited orlocalized chemical disorder is a common characteristic of the main matrix. Fundamentally different fromtraditional alloys, recently developed single-phase concentrated solid-solutio n alloys (CSAs) contain mul-tiple elemental species in equiatomic or high concentrations with different elements randomly arrangedon a crystalline lattice. Due to the lack of ordered elemental arrangement in these CSAs, they exhibit sig-nificant chemical disorder and unique site-to-site lattice distortion. While it is well recognized intraditional alloys that minor additions lead to enhanced radiation resistance, it remains unclear inCSAs how atomic-level heterogeneity affects defect formation, damage accumulation, and microstruc-tural evolution. These knowledge gaps have acted as roadblocks to the development of future-generation energy technology. CSAs with a simple crystal structure, but complex chemical disorder,are unique systems that allow us, through replacing principal alloying elements and modifying concen-trations, to study how compositional complexity influences defect dynamics, and to bridge the knowl-edge gaps through understanding intricate electronic- and atomic-level interactions, mass and energytransfer processes, and radiation resistance performance. Recent advances in defect dynamics and irradi-ation performance of CSAs are reviewed, intrinsic chemical effects on radiation performance arediscussed, and direction for future studies is suggested.
Level Alignment of a Prototypical Photocatalytic System: Methanol on TiO2(110)
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Observation of the continuous transformation of a four level laser into a two level system
A longstanding and fundamental question of laser and maser physics concerns the energy separation ({Delta}{epsilon}) required between the pumped and lasing states of a three (or four) level system. We observe a four level laser gradually transform into a two level (nonlasing) system by photoassociating Cs-Ar thermal atomic pairs and monitoring subsequent stimulated emission on the 6p{sup 2}P{sub 3/2} {yields} 6s{sup 2}S{sub 1/2} (D{sub 2}) transition of Cs at 852.1 nm. Laser excitation spectra demonstrate that the value of {Delta}{epsilon} below which the system rapidly assumes the form of a two level structure and lasing ceases is {approx}0.7kT which corresponds to a Boltzmann factor (exp[-{Delta}{epsilon}/kT]) of 0.5.
Magnetic-field-induced mixed-level Kondo effect in two-level systems
We consider a two-orbital impurity system with intra-and interlevel Coulomb repulsion that is coupled to a single conduction channel. This situation can generically occur in multilevel quantum dots or in systems of coupled quantum dots. For finite energy spacing between spin-degenerate orbitals, an in-plane magnetic field drives the system from a local-singlet ground state to a "mixed-level" Kondo regime, where the Zeeman-split levels are degenerate for opposite-spin states. We use the numerical renormalization group approach to fully characterize this mixed-level Kondo state and discuss its properties in terms of the applied Zeeman field, temperature, and system parameters. Under suitable conditions, the total spectral function is shown to develop a Fermi-level resonance, so that the linear conductance of the system peaks at a finite Zeeman field while it decreases as a function of temperature. These features, as well as the local moment and entropy contribution of the impurity system, are commensurate with Kondo physics, which can be studied in suitably tuned quantum dot systems.
Thermodynamic assessment of the hollandite high‐level radioactive waste form
Abstract Hollandite has been studied as a candidate ceramic waste form for the disposal of high‐level radioactive waste due to its inherent leach resistance and ability to immobilize alkaline‐earth metals such as Cs and Ba at defined lattice sites in the crystallographic structure. The chemical and structural complexity of hollandite‐type phases developed for high‐level waste immobilization limits the systematic experimental research that is required to understand phase development due to the large number of potential additives and compositional ranges that must be evaluated. Modeling the equilibrium behavior of the complex hollandite‐forming oxide waste system would aid in the design and processing of hollandite waste forms by predicting their thermodynamic stability. Thus, a BaO–Cs 2 O–TiO 2 –Cr 2 O 3 –Al 2 O 3 –Fe 2 O 3 –FeO–Ga 2 O 3 thermodynamic database was developed in this work according to the CALPHAD methodology. The compound energy formalism was used to model solid solution phases such as hollandite while the two‐sublattice partially ionic liquid model characterized the oxide melt. Results of model optimizations are presented and discussed including a 1473 K isothermal BaO–Cs 2 O–TiO 2 pseudo‐ternary diagram that extrapolates phase equilibrium behavior to regions not experimentally explored.
Homeostatic levels of nonstructural carbohydrates after 13 yr of drought and irrigation in Pinus sylvestris
Nonstructural carbohydrates (NSCs) are important for the growth and survival of trees. Drought may lead to a decrease in tree growth and to NSC depletion, whereas increased soil moisture in otherwise dry ecosystems may increase growth and NSC concentrations. A long-term (13 yr) irrigation experiment was conducted in a Pinus sylvestris-dominated forest located at the dry margin of the species in southern Switzerland. We measured the relative leaf area, growth, NSCs, needle d13C, [N] and [P] in trees on control and irrigated plots. Irrigation resulted in higher growth rates and carbon isotope discrimination, but did not alter NSC levels. Growth and NSC decreased with decreasing leaf area in both treatments, but NSC did not correlate with leaf-level gas exchange indices, such as foliar d13C, [N] or [P]. A legacy effect was shown, as trees with initially low leaf area had limited ability to respond to prolonged irrigation. The NSC constancy across treatments provides evidence that carbohydrate storage may stay constant when climate changes are sufficiently slow to allow acclimation. Moreover, we speculate that total leaf area, rather than leaf gas exchange per unit leaf area, drives the variation in whole-tree carbohydrate dynamics in this system.
Novel multimodality segmentation using level sets and Jensen-Rényi divergence
Purpose: Positron emission tomography (PET) is playing an increasing role in radiotherapy treatment planning. However, despite progress, robust algorithms for PET and multimodal image segmentation are still lacking, especially if the algorithm were extended to image-guided and adaptive radiotherapy (IGART). This work presents a novel multimodality segmentation algorithm using the Jensen-Rényi divergence (JRD) to evolve the geometric level set contour. The algorithm offers improved noise tolerance which is particularly applicable to segmentation of regions found in PET and cone-beam computed tomography. Methods: A steepest gradient ascent optimization method is used in conjunction with the JRD and a level set active contour to iteratively evolve a contour to partition an image based on statistical divergence of the intensity histograms. The algorithm is evaluated using PET scans of pharyngolaryngeal squamous cell carcinoma with the corresponding histological reference. The multimodality extension of the algorithm is evaluated using 22 PET/CT scans of patients with lung carcinoma and a physical phantom scanned under varying image quality conditions. Results: The average concordance index (CI) of the JRD segmentation of the PET images was 0.56 with an average classification error of 65%. The segmentation of the lung carcinoma images had a maximum diameter relative error of 63%, 19.5%, and 14.8% when using CT, PET, and combined PET/CT images, respectively. The estimated maximal diameters of the gross tumor volume (GTV) showed a high correlation with the macroscopically determined maximal diameters, with aR{sup 2} value of 0.85 and 0.88 using the PET and PET/CT images, respectively. Results from the physical phantom show that the JRD is more robust to image noise compared to mutual information and region growing. Conclusions: The JRD has shown improved noise tolerance compared to mutual information for the purpose of PET image segmentation. Presented is a flexible framework for multimodal image segmentation that can incorporate a large number of inputs efficiently for IGART.
On the determination of reference levels for quality assurance of flattening filter free photon beams in radiation therapy
Purpose: New definitions for some dosimetric parameters for use in quality assurance of flattening filter free (FFF) beams generated by medical linear accelerators have been suggested. The present study aims to validate these suggestions and to propose possible reference levels. Methods: The main characteristics of FFF photon beams were described in terms of: field size, penumbra, unflatness, slope, and peak-position parameters. Data were collected for 6 and 10 MV-FFF beams from three different Varian TrueBeam Linacs. Measurements were performed with a 2D-array (Starcheck system from PTW-Freiburg) and with the portal dosimetry method GLAaS utilizing the build-in portal imager of TrueBeam. Data were also compared to ion chamber measurements. A cross check validation has been performed on a FFF beam of 6 MV generated by a Varian Clinac-iX upgraded to FFF capability. Results : All the parameters suggested to characterize the FFF beams resulted easily measurable and little variation was observed among different Linacs. Referring to two reference field sizes of 10 × 10 and 20 × 20 cm{sup 2}, at SDD = 100 cm and d = dmax, from the portal dosimetry data, the following results (averaging X and Y profiles) were obtained. Field size: 9.95 ± 0.02 and 19.98 ± 0.03 cm for 6 MV-FFF (9.94 ± 0.02 and 19.98 ± 0.03 cm for 10 MV-FFF). Penumbra: 2.7 ± 0.3 and 2.9 ± 0.3 mm for 6 MV-FFF (3.1 ± 0.2 and 3.3 ± 0.3 for 10 MV-FFF). Unflatness: 1.11 ± 0.01 and 1.25 ± 0.01 for 6 MV-FFF (1.21 ± 0.01 and 1.50 ± 0.01 for 10 MV-FFF). Slope: 0.320 ± 0.020%/mm and 0.43 ± 0.015%/mm for 6 MV-FFF (0.657 ± 0.023%/mm and 0.795 ± 0.017%/mm for 10 MV-FFF). Peak Position −0.2 ± 0.2 and −0.4 ± 0.2 mm for 6 MV-FFF (−0.3 ± 0.2 and 0.7 ± 0.3 mm for 10 MV-FFF). Results would depend upon measurement depth. With thresholds set to at least 95% confidence level from the measured data and to account for possible variations between detectors and methods and experimental settings, a tolerance set of: 1 mm for field size and penumbra, 0.04 for unflatness, 0.1%/mm for slope, and 1 mm for peak position could be proposed from our data. Conclusions : The parameters proposed for the characterization and routine control of stability of profiles of FFF beams appear to be a viable solution with a strong similarity to the conventional parameters used for flattened beams. The results from three different TrueBeams and the cross-validation against a Clinac-iX suggested the possible generalization of the methods and the possibility to use common tolerances for the parameters. The data showed also the reproducibility of beam characteristics among different systems (of the same vendor) and the resulting parameter values could therefore be possibly generalized.
Numerical simulations of a transverse indirect circulation and low-level jet in the exit region of an upper-level jet
A numerical study was performed of a severe weather event (tornado) which occurred on May 10, 1973 in the Ohio region. The situation was modeled with a primitive equation mesoscale dynamic formulation. Account was taken of precipitation, the planetary boundary layer parameters as bulk quantities, the vertical pressure gradient, and lateral boundary conditions based on radiosonde data. Two 12-hr simulations, adiabatic and nondivergent, respectively, were analyzed for relationships between upper and lower level jets. In the adiabatic formulation, a transverse circulation with a low level jet formed at the exit region of the upper level jet. The nondivergent situation led to similar, but weaker, phenomena. Both forms suggest that indirect circulation in the exit zone of an upper level jet is strongly influenced by the initial structure of the jet.
Premature Deaths Due to Heat Exposure: the Potential Effects of Neighborhood-Level Versus City-Level Acclimatization Within Us Cities
For the population of a given US city, the risk of premature death associated with heat exposure increases as temperatures rise, but risks in hotter cities are generally lower than in cooler cities at equivalent temperatures due to factors such as acclimatization. Those living in especially hot neighborhoods within cities might therefore suffer much more than average if such adaptation is only at the city-wide level, whereas they might not experience greatly increased risk if adjustment is at the neighborhood level. To compare these possibilities, we use high spatial resolution temperature data to evaluated heat-related deaths assuming either adjustment at the city-wide or at the neighborhood scale in 10 large US cities. On average, we find that if inhabitants are adjusted to their local conditions, a neighborhood that was 10°C hotter than a cooler one would experience only about 1.0–1.5 excess heat deaths per year per 100,000 persons. By contrast, if inhabitants are acclimatized to city-wide temperatures, the hotter neighborhood would experience about 15 excess deaths per year per 100,000 persons. Using idealized analyses, we demonstrate that current city-wide epidemiological data do not differentiate between these differing adjustments. Given the very large effects of assumptions about neighborhood-level acclimatization found here, as well as the fact that current literature is conflicting on the spatial scale of acclimatization, more neighborhood-level epidemiological data are urgently needed to determine the health impacts of variations in heat exposure within urban areas, better constrain projected changes, and inform mitigation efforts.
Resolving the EH{sub 6/7} level in 4H-SiC by Laplace-transform deep level transient spectroscopy
We show that Laplace transform deep level transient spectroscopy (LDLTS) is an effective technique for the separation of the overlapping emission rates of the EH{sub 6} and EH{sub 7} levels, which are known to constitute EH{sub 6/7}, a mid-gap level in n-type 4H-SiC. The analysis of the electron irradiation dose, electric field dependence, and the effects of carbon interstitials injection on the emission rates of EH{sub 6} and EH{sub 7} shows that EH{sub 7} is dominant over EH{sub 6} and confirms that their nature is related to a carbon vacancy.
Quasi-Fermi level splitting and sub-bandgap absorptivity from semiconductor photoluminescence
A unified model for the direct gap absorption coefficient (band-edge and sub-bandgap) is developed that encompasses the functional forms of the Urbach, Thomas-Fermi, screened Thomas-Fermi, and Franz-Keldysh models of sub-bandgap absorption as specific cases. We combine this model of absorption with an occupation-corrected non-equilibrium Planck law for the spontaneous emission of photons to yield a model of photoluminescence (PL) with broad applicability to band-band photoluminescence from intrinsic, heavily doped, and strongly compensated semiconductors. The utility of the model is that it is amenable to full-spectrum fitting of absolute intensity PL data and yields: (1) the quasi-Fermi level splitting, (2) the local lattice temperature, (3) the direct bandgap, (4) the functional form of the sub-bandgap absorption, and (5) the energy broadening parameter (Urbach energy, magnitude of potential fluctuations, etc.). The accuracy of the model is demonstrated by fitting the room temperature PL spectrum of GaAs. It is then applied to Cu(In,Ga)(S,Se){sub 2} (CIGSSe) and Cu{sub 2}ZnSn(S,Se){sub 4} (CZTSSe) to reveal the nature of their tail states. For GaAs, the model fit is excellent, and fitted parameters match literature values for the bandgap (1.42 eV), functional form of the sub-bandgap states (purely Urbach in nature), and energy broadening parameter (Urbach energy of 9.4 meV). For CIGSSe and CZTSSe, the model fits yield quasi-Fermi leveling splittings that match well with the open circuit voltages measured on devices made from the same materials and bandgaps that match well with those extracted from EQE measurements on the devices. The power of the exponential decay of the absorption coefficient into the bandgap is found to be in the range of 1.2 to 1.6, suggesting that tunneling in the presence of local electrostatic potential fluctuations is a dominant factor contributing to the sub-bandgap absorption by either purely electrostatic (screened Thomas-Fermi) or a photon-assisted tunneling mechanism (Franz-Keldysh). A Gaussian distribution of bandgaps (local E{sub g} fluctuation) is found to be inconsistent with the data. The sub-bandgap absorption of the CZTSSe absorber is found to be larger than that for CIGSSe for materials that yield roughly equivalent photovoltaic devices (8% efficient). Further, it is shown that fitting only portions of the PL spectrum (e.g., low energy for energy broadening parameter and high energy for quasi-Fermi level splitting) may lead to significant errors for materials with substantial sub-bandgap absorption and emission.
Deep levels in as-grown and electron-irradiated n-type GaN studied by deep level transient spectroscopy and minority carrier transient spectroscopy
Development of high performance GaN-based devices is strongly dependent on the possibility to control and understand defects in material. Important information about deep level defects is obtained by deep level transient spectroscopy and minority carrier transient spectroscopy on as-grown and electron irradiated n-type bulk GaN with low threading dislocation density produced by halide vapor phase epitaxy. One hole trap labelled H1 (E{sub V} + 0.34 eV) has been detected on as-grown GaN sample. After 2 MeV electron irradiation, the concentration of H1 increases and at fluences higher than 5 × 10{sup 14 }cm{sup −2}, a second hole trap labelled H2 is observed. Simultaneously, the concentration of two electron traps, labelled T1 (E{sub C} – 0.12 eV) and T2 (E{sub C} – 0.23 eV), increases. By studying the increase of the defect concentration versus electron irradiation fluence, the introduction rate of T1 and T2 using 2 MeV- electrons was determined to be 7 × 10{sup −3 }cm{sup −1} and 0.9 cm{sup −1}, respectively. Due to the low introduction rate of T1, it is suggested that the defect is associated with a complex. The high introduction rate of trap H1 and T2 suggests that the defects are associated with primary intrinsic defects or complexes. Some deep levels previously observed in irradiated GaN layers with higher threading dislocation densities are not detected in present investigation. It is therefore suggested that the absent traps may be related to primary defects segregated around dislocations.
High-spin level structure of {sup 115}Rh: Evolution of triaxiality in odd-even Rh isotopes
High-spin excited states in the neutron-rich nucleus {sup 115}Rh have been identified for the first time by studying prompt {gamma} rays from the spontaneous fission of {sup 252}Cf with the Gammasphere detector array. A new yrast band and a sideband are built in {sup 115}Rh. This level scheme is proposed to be built on the 7/2{sup +} ground state. The existence of a large signature splitting and an yrare band in {sup 115}Rh shows typical features of a triaxially deformed nucleus. The rigid triaxial rotor plus particle model is used to interpret the level structure of {sup 115}Rh. The level energies, the {gamma} branching ratios, the large signature splitting in the yrast band, and the inverted signature splitting in the yrare band in {sup 115}Rh are reproduced very well. Strong K mixing occurs in {sup 115}Rh at high spin.