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All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Enhanced Thermoelectric Properties of Heavy-fermion Compounds $\text{Yb}_x\text{Ce}_y\text{Sm}_z\text{Ir}_2\text{Zn}_{20}$ $(x+y+z=1)$

Herein, thermoelectric materials hold tremendous promise for advances in fundamental science and practical ap- plications, particularly for robust electricity generation in extreme and remote environments. Despite this, for most materials the energy conversion efficiency is limited by the proportionality between the electrical and thermal conductivities and small values of the Seebeck coefficient for metals. It was previously reported that the heavy-fermion compound $\text{YbIr}_2$ $\text{Zn}_{20}$ exhibits large Seebeck coefficient and thermoelectric figure of merit $ZT$ at 35 K. This behavior is primarily associated with strong hybridization between the $f$- and conduction electron states. Here, we seek to improve the thermoelectric properties through chemical substitution on the Yb site using Ce and Sm. By surveying different levels of substitution, we find that the thermoelectric properties vary strongly with the $f$-element ratio. This confirms that electronic hybridization dominates the thermoelectric properties and clarifies directions for optimizing these materials for applications. We also investigate the impact of the disorder on the thermal conductivity, where we find only weak variation with lanthanide content.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Sequential infiltration of two-photon polymerized 3D photonic crystals for mid-IR spectroscopic applications

Photonic crystals (PhCs) are spatially organized structures with lattice parameters equivalent to the operational wavelength of light. PhCs have been subject to extensive research efforts in the last two decades and are known for controlling light propagation with applications in sensing and time-delayed communication due to the slow-light phenomenon. Despite their exceptional properties, PhCs are difficult to fabricate using planar micromachining techniques due to their periodic structures. Techniques like two-photon stereolithography have been discussed for PhC fabrication in the literature, but the inherent disadvantage of poor refractive index (RI) contrast results in limited application. In this work, we present sequential infiltration synthesis performed on two-photon stereolithographically printed 3D PhCs for infiltration with zinc oxide to increase the RI of 3D PhCs. Further, finite element analysis was performed over a range of RI contrast values to study the change in photonic bandgap (PBG) with RI contrast. The transmission spectra were recorded on 3D PhCs before and after infiltration to demonstrate the change experimentally. An increase in the PBG width and absorbance is seen postinfiltration due to enhanced RI. This work presents the first, to our knowledge, sequentially infiltrated enhanced 3D PhC fabricated with two-photon stereolithography.

3D printing↗
DOE OSTI2016

Experimental Effects on IR Reflectance Spectra: Particle Size and Morphology

For geologic and extraterrestrial samples it is known that both particle size and morphology can have strong effects on the species’ infrared reflectance spectra. Due to such effects, the reflectance spectra cannot be predicted from the absorption coefficients alone. This is because reflectance is both a surface as well as a bulk phenomenon, incorporating both dispersion as well as absorption effects. The same spectral features can even be observed as either a maximum or minimum. The complex effects depend on particle size and preparation, as well as the relative amplitudes of the optical constants n and k, i.e. the real and imaginary components of the complex refractive index. While somewhat oversimplified, upward-going amplitude in the reflectance spectrum usually result from surface scattering, i.e. rays that have been reflected from the surface without penetration, whereas downward-going peaks are due to either absorption or volume scattering, i.e. rays that have penetrated or refracted into the sample interior and are not reflected. While the effects are well known, we report seminal measurements of reflectance along with quantified particle size of the samples, the sizing obtained from optical microscopy measurements. The size measurements are correlated with the reflectance spectra in the 1.3 – 16 micron range for various bulk materials that have a combination of strong and weak absorption bands in order to understand the effects on the spectral features as a function of the mean grain size of the sample. We report results for both sodium sulfate Na2SO4 as well as ammonium sulfate (NH4)2SO4; the optical constants have been measured for (NH4)2SO4. To go a step further from the field to the laboratory we explore our understanding of particle size effects on reflectance spectra in the field using standoff detection. This has helped identify weaknesses and strengths in detection using standoff distances of up 160 meters away from the Target. The studies have shown that particle size has an enormous influence on the measured reflectance spectra of such materials; successful identification requires sufficient, representative reflectance data to include the particle sizes of interest.

Beiswenger, Toya N.↗
DOE OSTI2012

Heteroleptic cyclometalated Ir(III) complexes with charge transporting groups: A theoretical study

Efficient and stable high energy organic light emitting devices (OLEDs) are a vital component of new generation general illumination solutions. However, large charge imbalances in the emissive layer of OLEDs lead to charge accumulation and subsequent side reactions which lowers the device efficiency and dramatically shortens operational lifetime. Radical changes in the way emitter materials are designed are needed to address this problem. Conventional approaches have only focused on color tuning; however, multi-functional emitter materials are needed to assist the transport of charge in the emissive layer. We propose to design and synthesize new organometallic iridium phosphorescent materials with bipolar charge transport properties to be used in high energy OLEDs and white light configurations

Organic light emitting devices, rational design, o↗
DOE OSTI2013

Dosimetric accuracy of a deterministic radiation transport based {sup 192}Ir brachytherapy treatment planning system. Part III. Comparison to Monte Carlo simulation in voxelized anatomical computational models

Purpose: To compare TG43-based and Acuros deterministic radiation transport-based calculations of the BrachyVision treatment planning system (TPS) with corresponding Monte Carlo (MC) simulation results in heterogeneous patient geometries, in order to validate Acuros and quantify the accuracy improvement it marks relative to TG43. Methods: Dosimetric comparisons in the form of isodose lines, percentage dose difference maps, and dose volume histogram results were performed for two voxelized mathematical models resembling an esophageal and a breast brachytherapy patient, as well as an actual breast brachytherapy patient model. The mathematical models were converted to digital imaging and communications in medicine (DICOM) image series for input to the TPS. The MCNP5 v.1.40 general-purpose simulation code input files for each model were prepared using information derived from the corresponding DICOM RT exports from the TPS. Results: Comparisons of MC and TG43 results in all models showed significant differences, as reported previously in the literature and expected from the inability of the TG43 based algorithm to account for heterogeneities and model specific scatter conditions. A close agreement was observed between MC and Acuros results in all models except for a limited number of points that lay in the penumbra of perfectly shaped structures in the esophageal model, or at distances very close to the catheters in all models. Conclusions: Acuros marks a significant dosimetry improvement relative to TG43. The assessment of the clinical significance of this accuracy improvement requires further work. Mathematical patient equivalent models and models prepared from actual patient CT series are useful complementary tools in the methodology outlined in this series of works for the benchmarking of any advanced dose calculation algorithm beyond TG43.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2014

WE-A-17A-08: Evaluation of the OncentraBrachy Collapsed Cone Convolution Algorithm for Ir-192 Source Using Phantom and Real-Patient Heterogeneous Geometries

Purpose: To evaluate the commercially released Collapsed Cone convolution-based(CCC) dose calculation module of the Elekta OncentraBrachy(OcB) treatment planning system(TPS). Methods: An allwater phantom was used to perform TG43 benchmarks with single source and seventeen sources, separately. Furthermore, four real-patient heterogeneous geometries (chestwall, lung, breast and prostate) were used. They were selected based on their clinical representativity of a class of clinical anatomies that pose clear challenges. The plans were used as is(no modification). For each case, TG43 and CCC calculations were performed in the OcB TPS, with TG186-recommended materials properly assigned to ROIs. For comparison, Monte Carlo simulation was run for each case with the same material scheme and grid mesh as TPS calculations. Both modes of CCC (standard and high quality) were tested. Results: For the benchmark case, the CCC dose, when divided by that of TG43, yields hot-n-cold spots in a radial pattern. The pattern of the high mode is denser than that of the standard mode and is representative of angular dicretization. The total deviation ((hot-cold)/TG43) is 18% for standard mode and 11% for high mode. Seventeen dwell positions help to reduce “ray-effect”, with the total deviation to 6% (standard) and 5% (high), respectively. For the four patient cases, CCC produces, as expected, more realistic dose distributions than TG43. A close agreement was observed between CCC and MC for all isodose lines, from 20% and up; the 10% isodose line of CCC appears shifted compared to that of MC. The DVH plots show dose deviations of CCC from MC in small volume, high dose regions (>100% isodose). For patient cases, the difference between standard and high modes is almost undiscernable. Conclusion: OncentraBrachy CCC algorithm marks a significant dosimetry improvement relative to TG43 in real-patient cases. Further researches are recommended regarding the clinical implications of the above observations. Support provided by a CIHR grant and CCC system provided by Elekta-Nucletron.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2016

Therapeutic analysis of high-dose-rate {sup 192}Ir vaginal cuff brachytherapy for endometrial cancer using a cylindrical target volume model and varied cancer cell distributions

Purpose: To evaluate high-dose-rate (HDR) vaginal cuff brachytherapy (VCBT) in the treatment of endometrial cancer in a cylindrical target volume with either a varied or a constant cancer cell distributions using the linear quadratic (LQ) model. Methods: A Monte Carlo (MC) technique was used to calculate the 3D dose distribution of HDR VCBT over a variety of cylinder diameters and treatment lengths. A treatment planning system (TPS) was used to make plans for the various cylinder diameters, treatment lengths, and prescriptions using the clinical protocol. The dwell times obtained from the TPS were fed into MC. The LQ model was used to evaluate the therapeutic outcome of two brachytherapy regimens prescribed either at 0.5 cm depth (5.5 Gy × 4 fractions) or at the vaginal mucosal surface (8.8 Gy × 4 fractions) for the treatment of endometrial cancer. An experimentally determined endometrial cancer cell distribution, which showed a varied and resembled a half-Gaussian distribution, was used in radiobiology modeling. The equivalent uniform dose (EUD) to cancer cells was calculated for each treatment scenario. The therapeutic ratio (TR) was defined by comparing VCBT with a uniform dose radiotherapy plan in term of normal cell survival at the same level of cancer cell killing. Calculations of clinical impact were run twice assuming two different types of cancer cell density distributions in the cylindrical target volume: (1) a half-Gaussian or (2) a uniform distribution. Results: EUDs were weakly dependent on cylinder size, treatment length, and the prescription depth, but strongly dependent on the cancer cell distribution. TRs were strongly dependent on the cylinder size, treatment length, types of the cancer cell distributions, and the sensitivity of normal tissue. With a half-Gaussian distribution of cancer cells which populated at the vaginal mucosa the most, the EUDs were between 6.9 Gy × 4 and 7.8 Gy × 4, the TRs were in the range from (5.0){sup 4} to (13.4){sup 4} for the radiosensitive normal tissue depending on the cylinder size, treatment lengths, prescription depth, and dose as well. However, for a uniform cancer cell distribution, the EUDs were between 6.3 Gy × 4 and 7.1 Gy × 4, and the TRs were found to be between (1.4){sup 4} and (1.7){sup 4}. For the uniformly interspersed cancer and radio-resistant normal cells, the TRs were less than 1. The two VCBT prescription regimens were found to be equivalent in terms of EUDs and TRs. Conclusions: HDR VCBT strongly favors cylindrical target volume with the cancer cell distribution following its dosimetric trend. Assuming a half-Gaussian distribution of cancer cells, the HDR VCBT provides a considerable radiobiological advantage over the external beam radiotherapy (EBRT) in terms of sparing more normal tissues while maintaining the same level of cancer cell killing. But for the uniform cancer cell distribution and radio-resistant normal tissue, the radiobiology outcome of the HDR VCBT does not show an advantage over the EBRT. This study strongly suggests that radiation therapy design should consider the cancer cell distribution inside the target volume in addition to the shape of target.

61 RADIATION PROTECTION AND DOSIMETRY↗
DOE OSTI2016

WE-DE-201-10: Pitfalls When Using Ruby as An Inorganic Scintillator Detector for Ir-192 Brachytherapy Dosimetry

Purpose: To study the promising potential of inorganic scintillator detectors (ISDs) and investigate various unwanted luminescence properties which may compromise their accuracy. Methods: The ISDs were comprised of a ruby crystal coupled to a polymethyl methacrylate (PMMA) fiber-optic cable and a charged coupled device camera. A new type of ISD was manufactured and included a long-pass filter that was sandwiched between the crystal and the fiber-optic cable. The purpose of the filter was to suppress the Cerenkov and fluorescence background light induced in the PMMA (the stem signal) from striking the ruby crystal, generating unwanted ruby excitation. A variety of experiments were performed to characterize the ruby based ISDs. The relative contribution of the induced ruby signal and the stem signal were quantified while exposing the detector and a bare fiber-optic cable to a high dose rate (HDR) brachytherapy (BT) source, respectively. The unwanted ruby excitation was quantified while irradiating the fiber-optic cable with the detector volume shielded. Other experiments addressed time-dependent luminescence properties and a comparison to other commonly used organic scintillator detectors (BCF-12, BCF-60). Results: When the BT source dwelled 0.5 cm away from the fiber-optic cable, the unwanted ruby excitation amounted to >5% of the total signal if the source-distance from the scintillator was >7 cm. However, the unwanted excitation was suppressed to <1% if the ISD incorporated an optic filter. The stem signal was suppressed with a 20 nm band-pass filter and was <3% as long as the source-distance was <7 cm. The ruby based ISDs generated signal up to 20(40) times that of BCF-12(BCF-60). Conclusion: The study presents solutions to unwanted luminescence properties of ruby based ISDs for HDR BT. An optic filter should be sandwiched between the scintillator volume and the fiber-optic cable to prevent the stem signal to excite the ruby crystal.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗