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High-Performance Flexible Bismuth Telluride Thin Film from Solution Processed Colloidal Nanoplates
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Lead Telluride Nanowires for Surface Passivation in Cadmium Telluride Photovoltaics
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Pyrolyzer Assisted Vapor Transport Deposition of Antimony-Doped Cadmium Telluride
In this study, we developed a new method for in situ Sb doping of CdTe thin films combining vapor transport deposition with a Group V pyrolyzer to address Sb doping concentration and doping efficiency. The Sb doped CdSeTe (CdSeTe:Sb) films were deposited in solar cell structures under variations of Sb dopant source heater, vapor pyrolyzer temperature, and Cd vapor excess. Results indicate that although these parameters do not affect the CdTe morphology or crystal structure, they critically influence doping efficiency and trap concentration. Capacitance-voltage measurements show that a higher dopant heater (TD) or pyrolyzer (TP) temperature leads to higher net carrier concentration, achieving a net carrier concentration of 1016 cm-3 and 20% doping efficiency with a TD/TP combination of 600 degrees C/1100 degrees C. By tuning the Cd/Sb flux ratio during CdSeTe:Sb deposition, the lowest defect concentration is achieved at Cd/Sb of 1.4:1, which produced the best VOC CdSeTe:Sb cell. This demonstrates a path to produce high net carrier concentration polycrystalline CdTe thin film with a low concentration of dopant-induced defects.
Structural Design of Bismuth Telluride Nanoplates through Process Variables
Binary pnictogen chalcogen compounds, primarily bismuth tellurides and selenides, are of great interest due to their applications in emerging quantum devices, as well as thermoelectric generators. The performance of bismuth telluride in these roles depends on its structure at the nanoscale, particularly the size, shape, and crystallinity of its nanocrystalline forms. However, current methods for controlling these features are often slow, inconsistent, or difficult to scale. Here, we demonstrate that through a solvothermal synthesis and hot injection process, precise control over the morphology of bismuth telluride nanoplates is possible with independent tuning of process variables, such as temperature and reaction time. We find that the nanoplate shape and internal porosity vary systematically with synthesis temperature and that the same morphological outcomes can be rapidly achieved at a fixed temperature by adjusting reaction duration. These results reveal that both the temperature and time can independently direct bismuth telluride morphological features, allowing for rapid, tunable synthesis strategies. Our approach offers a scalable framework, not only for bismuth telluride but also for related layered chalcogenides used in energy harvesting and quantum technologies.
Freeform thermoelectrics in single-step manufacturing: additive manufacturing of bismuth-telluride thermoelectrics
The project succeeded in producing crack-free Bismuth Telluride thermoelectric parts with density exceeding 98% through laser powder bed fusion (LPBF) additive manufacturing (AM). This greatly exceeded the highest previously reported density of 88% and is the highest among all semiconducting materials processed by LPBF. The additively manufactured material shows comparable Seebeck coefficient as conventional form and can be made into complex geometries with reduced material loss. On the other hand, measured properties are dramatically sensitive to the AM process parameters used, such that with identical composition, the Seebeck coefficient can be controllably tuned from +120 µV/K to -207 µV/K, which means the material switches between an n-type to a p-type semiconductor depending on processing. These changes are accompanied by significant differences in the as-processed microstructure due to rapid solidification. A machine learning protocol was developed and greatly reduced the experimental burden of the project, reducing the typical process optimization period of 2 years to 6 months. The project was fully successful in the objective of producing defect-free, complex geometry of bismuth-telluride parts through LPBF, but only partially successful in achieving performance goals. First, cost reduction of manufacturing, as measured by material waste, was successfully reduced by up to 70% compared to conventional manufacturing methods. This exceeded the proposed 30% reduction in materials waste needed to reach the 20% cost reduction goal of the project. On the other hand, the device performance, as measured by Seebeck coefficient, failed to reach the 40% improvement in efficiency. Rather, we observe comparable Seebeck coefficient between AM samples and conventionally processed counterparts. The device-level efficiency improvement does exceed 40% for complex geometry samples due to shape-induced increase in temperature gradients, but this was not the originally proposed metric. The machine learning approach developed in this project greatly accelerated the process optimization and can be adopted for fast development of AM processing parameters for other brittle and otherwise difficult-to-print materials. For the public, we deliver an efficient and widely adoptable process for incorporating waste-heat harvesting thermoelectric devices in both industrial and commercial heat exchangers. The geometric flexibility allows the capturing device to conform to the shape of the heat source to improve the system-level conversion efficiency. The technique can be deployed on any commercial LBPF systems with zero modifications, thus poses minimal adoption barrier for any manufacturer that already employed AM technology. Beyond bismuth-telluride, the machine-learning guided optimization protocol can be used in the future to reduce both the time and cost of process development for AM of other energy conversion and harvesting materials.
Ex Situ Photoelectron Emission Microscopy of Polycrystalline Bismuth and Antimony Telluride Surfaces Exposed to Ambient Oxidation
The surfaces of textured polycrystalline N-type bismuth telluride and P-type antimony telluride materials were investigated using ex situ photoelectron emission microscopy (PEEM). PEEM enabled imaging of the work function for different oxidation times due to exposure to air across sample surfaces. The spatially averaged work function was also tracked as a function of air exposure time. N-type bismuth telluride showed an increase in the work function around grain boundaries relative to grain interiors during the early stages of air exposure-driven oxidation. At longer time exposure to air, the surface became homogenous after a ~5 nm-thick oxide formed. X-ray photoemission spectroscopy was used to correlate changes in PEEM imaging in real space and work function evolution to the progressive growth of an oxide layer. The observed work function contrast is consistent with the pinning of electronic surface states due to the defects at a grain boundary.
Pulsed laser deposition assisted epitaxial growth of cesium telluride photocathodes for high brightness electron sources
The development of high-brightness electron sources is critical to state-of-the-art electron accelerator applications like X-ray free electron laser (XFEL) and ultra-fast electron microscopy. Cesium telluride is chosen as the electron source material for multiple cutting-edge XFEL facilities worldwide. This manuscript presents the first demonstration of the growth of highly crystalized and epitaxial cesium telluride thin films on 4H-SiC and graphene/4H-SiC substrates with ultrasmooth film surfaces. The ordering of the film was characterized by in situ reflection high energy electron diffraction and multiple X-ray diagnostics. The results of the quantum efficiency performance for epitaxial cesium telluride photocathodes are also reported.
Magnetocaloric effect observations near room temperature in few-layered chromium telluride (Cr 2 Te 3 )
Transition metal telluride compositions are explored extensively for their unique magnetic behavior. Few-layered chromium telluride (Cr 2 T e3 ) exhibits a near-room-temperature phase transition, where the material can be effectively used in applications such as magnetic refrigeration. Compared to existing magnetocaloric materials, Heusler alloys, and rare-earth-based alloys, the large-scale synthesis of mechanically exfoliated Cr 2 Te 3 involves less complexity, resulting in a stable composition. Compared to existing tellurides, Cr 2 Te 3 exhibited a large change in magnetic entropy (|ΔS M |) of 1.88 J k g−1 K −1 at a magnetic field of 4 T. A refrigeration capacity (RC) of ∼82 J kg −1 was determined from the change in magnetic entropy versus temperature curve. The results were comparable with those for existing Cr-based compounds. First-principles density functional theory (DFT) confirmed the magnetic properties of Cr 2 Te 3 , including a near-room-temperature Curie temperature, T C , consistent with experimental results. Here, structural transition was also observed using first-principles DFT, which is responsible for the magnetic behavior.
Oxygen isotope evidence for input of magmatic fluids and precipitation of Au-Ag-tellurides in an otherwise ordinary adularia-sericite epithermal system in NE China
Abstract Tellurium-rich (Te) adularia-sericite epithermal Au-Ag deposits are an important current and future source of precious and critical metals. However, the source and evolution of ore-forming fluids in these deposits are masked by traditional bulk analysis of quartz oxygen isotope ratios that homogenize fine-scale textures and growth zones. To advance understanding of the source of Te and precious metals, herein, we use petrographic and cathodoluminescence (CL) images of such textures and growth zones to guide high spatial resolution secondary ion mass spectroscopy (SIMS) oxygen isotope analyses (10 µm spot) and spatially correlated fluid inclusion microthermometric measurements on successive quartz bands in contemporary Te-rich and Te-poor adularia-sericite (-quartz) epithermal Au-Ag vein deposits in northeastern China. The results show that large positive oxygen isotope shifts from –7.1 to +7.7‰ in quartz rims are followed by precipitation of Au-Ag telluride minerals in the Te-rich deposit, whereas small oxygen isotope shifts of only 4‰ (–2.2 to +1.6‰) were detected in quartz associated with Au-Ag minerals in the Te-poor deposits. Moreover, fluid-inclusion homogenization temperatures are higher in comb quartz rims (avg. 266.4 to 277.5 °C) followed by Au-Ag telluride minerals than in previous stages (~250 °C) in the Te-rich deposit. The Te-poor deposit has a consistent temperature (~245 °C) in quartz that pre- and postdates Au-Ag minerals. Together, the coupled increase in oxygen isotope ratios and homogenization temperatures followed by precipitation of Au-Ag tellurides strongly supports that inputs of magmatic fluid containing Au, Ag, and Te into barren meteoric water-dominated flow systems are critical to the formation of Te-rich adularia-sericite epithermal Au-Ag deposits. In contrast, Te-poor adularia-sericite epithermal Au-Ag deposits show little or no oxygen isotope or fluid-inclusion evidence for inputs of magmatic fluid.
Cadmium Magnesium Telluride for Next Generation X-Ray Free Electron Laser, Synchrotron and Many Other Applications
We developed a picosecond photodetector based on our Bridgman grown and specially engineered Cadmium Magnesium Telluride (Cd 1-x Mg x Te) single crystal that is sensitive to both optical and x-ray pulses for coarse timing in Free Electron Laser applications. Cd 1-x Mg x Te is a wide bandgap semiconductor material with potential applications, not only in optoelectronics, but also in particle physics as an intense pulse radiation detector for bremsstrahlung, X-ray/gamma ray radiation, thermal neutrons, and medical imaging. However, for femtosecond optical and x-ray cross correlation, the material has to have very short lifetime, a condition that is opposite to that required for nuclear spectroscopy applications. At the same time, the material also needs to have very low bulk leakage current, in the 0.10 pA range. Hence the ability to tailor or engineer the material is very crucial. In this paper, picosecond response and the crystal growth of this specially engineered cadmium magnesium telluride material will be presented. Other material characterization and transient measurements will also be discussed along with room temperature semiconductor detector performance for other nuclear radiation detection applications.
Effects of excess Te on flux inclusion formation in the growth of cadmium zinc telluride when forced melt convection is applied
The presence of second phase defects, particularly flux inclusions of tellurium rich composition, are of great concern for charge collection efficiency in cadmium zinc telluride (CZT) and cadmium telluride (CT) material intended for applications such as radiation detection. These inclusions can distort applied electric field lines within the detector as well as act as trapping centers for charge carriers. Reduction and/or elimination of these inclusions is required to achieve appropriate charge collection efficiencies, especially in detectors of thicknesses greater than 5 mm. These so-called flux inclusions are understood to form as a consequence of constitutional undercooling at the crystal growth interface. In this study, a forced melt convection technique was applied in Vertical Bridgman (VB) melt growth of CZT without reducing imposed growth rates of ~2 mm/hr. Several rotation profiles were tested while adjusting the melt composition from 51.62 to 61.75 atomic percent (at%) Te where the Te concentration was initially increased to improve overall material purity. With forced melt convection, the best inclusion distributions were achieved with highly Te rich melt compositions, far beyond the stoichiometric composition range for the CZT system. Average inclusion diameters were reduced to 2 µm while inclusions greater than 5 µm were essentially eliminated. Composition analyses of these ingots revealed near equilibrium concentrations of Te, even with ingots grown from Te concentrations as high as 61.75 at% Te. In this paper, a recipe for the reduction of inclusions in CZT melt growth is put forward and the implications of this method on our understanding of inclusion formation are discussed.
A Ba 6 Cu 31 Te 22 ( A = K, Rb, Cs) Featuring Polyanionic Copper–Telluride Frameworks with Ultralow Thermal Conductivity
In this study, hree polyanionic tellurides, ABa 6 Cu 31 Te 22 (A = K, Rb, Cs), were synthesized in salt flux. The isostructural tellurides crystallize in a new structure type, in the cubic Pa$\overline{3}$ space group with a Wyckoff sequence of d 10 c 2 b 1 and large unit cell volumes of over 5500 Å 3 . The structures feature a framework of [CuTe 4 ] tetrahedra and [CuTe 3 ] trigonal pyramids with disorder in the Cu sites. The polyanionic frameworks have large square antiprism and cuboctahedral voids where Ba and alkali metal cations are situated, forming [BaTe 8 ] and [ATe 12 ], respectively. The overall compositions are close to being charge balanced. The large [ATe 12 ] cuboctahedra allowed for significant anisotropic displacement of the A cations, as observed from both single crystal X-ray diffraction and heat capacity studies. Alkali cations rattling together with Cu atom displacement and disorder leads to the dispersion of phonons, thus softening the lattice and subsequently reducing the thermal conductivity. Evaluations of the electronic band structure revealed the occurrence of a narrow bandgap together with the presence of a flat band near the valence band maximum, giving rise to the high thermopower. The Cs and Rb analogues show a slope change in the temperature dependence of electrical resistivity around room temperature, which is typical for semimetals or degenerate semiconductors. For the as-synthesized and unoptimized materials, high values of the thermoelectric figure-of-merit of ~0.2 were observed at 623 K.
Monolayer 2D semiconducting tellurides for high-mobility electronics
Discovery and design of two-dimensional (2D) materials with suitable band gaps and high carrier mobility are of vital importance for the photonics, optoelectronics, and high-speed electronics. In this work, based on first principles calculations using density functional theory with Perdew-Burke-Ernzerhof and Heyd-Scuseria-Ernzerhoffunctionals, we introduce a family of monolayer isostructural semiconducting tellurides MNTe 4 , with M={Ti,Zr,Hf} and N={Si,Ge}. We find that these compounds have been identified to possess direct band gaps from 1.0 to 1.31 eV, which are well suited for photonics and optoelectronics applications. Additionally, anisotropic in-plane transport behavior is observed, and small electron and hole (0.11–0.15m e ) effective masses are identified along the dominant transport direction. Ultrahigh carrier mobility is predicted for this family of 2D compounds, which host great promise for potential applications in high-speed electronic devices. Furthermore, detailed analysis of electronic structures reveals the origins of the promising properties of this unique class of 2D telluride materials.
A Density Functional Theory (DFT) Study on the Effect of Chlorine in the Magnesium Zinc Oxide (MZO) Front Interface for Cadmium Telluride (CdTe) Thin Film Solar Cells
Cadmium telluride photovoltaics has benefitted greatly from the cadmium chloride treatment which causes a remarkable improvement in cell efficiencies. This work investigates the effect of elemental chlorine at the interface between the magnesium zinc oxide front contact and the cadmium telluride absorber in such a device. Band alignment including band bending and interface states and its role in potential charge carrier transport is the key feature studied. It is seen that a small amount of chlorine is leads to a more desirable band alignment. Higher concentrations of chlorine result in unfavorable band characteristics.
Cadmium Telluride Accelerator Consortium (CTAC)
The United States is the leader in cadmium telluride (CdTe) photovoltaic (PV) manufacturing, and CdTe is the second most-deployed solar technology in the world. The CdTe Accelerator Consortium (CTAC) was formed to enhance U.S. technology leadership and competitiveness in CdTe photovoltaics (PV) including increasing cell efficiencies, decreasing module costs, and maintaining or increasing domestic CdTe PV material and module production. Leadership for the 3-year consortium was selected by an NREL team through a competitive solicitation. CTAC was formally announced on August 1st by U.S. Secretary of Energy Jennifer M. Granholm and U.S. Representative Marcy Kaptur at an event held at University of Toledo. We will give an overview of CTAC research directions along with their goals and activities. We can also discuss how CTAC relates to the National Renewable Energy Laboratory (NREL) and to the U.S. Manufacturing of Advanced Cadmium Telluride Photovoltaics Consortium (US-MAC). Visit our poster to find out who leads CTAC and how you can get involved.
Germanium Telluride Chalcogenide Switches for RF Applications
This project developed prototype germanium telluride switches, which can be used in RF applications to improve SWAP (size, weight, and power) and signal quality in RF systems. These switches can allow for highly reconfigurable systems, including antennas, communications, optical systems, phased arrays, and synthetic aperture radar, which all have high impact on current National Security goals for improved communication systems and communication technology supremacy. The final result of the project was the demonstration of germanium telluride RF switches, which could act as critical elements necessary for a single chip RF communication system that will demonstrate low SWAP and high reconfigurability
Dynamically Tunable Terahertz Emission Enabled by Anomalous Optical Phonon Responses in Lead Telluride
Lead telluride (PbTe), a narrow bandgap semiconductor commonly used in infrared detectors, exhibits anomalous vibrational and structural properties, making it appealing for thermoelectrics. Despite significant fundamental interest in the microscopic origins of its unusual vibrational properties, the optical functionalities stemming from phonons and electron–phonon coupling in PbTe have not been closely investigated. This work reports measurements of terahertz (THz) radiation from a PbTe single crystal following ultrafast optical excitation and investigates IR-active phonon responses as a function of excitation fluence and temperature. We uncover a spectrally tunable THz emission peak enabled by an epsilon-near-zero response of the coupled plasmon–longitudinal optical phonon mode that can be dynamically shifted via tuning photocarrier density. Spectral tunability (Δω/ω = 25%) is significant and beyond what has been achieved by any other THz emitter. In addition, the emitted THz fields reveal signatures of a zone center transverse optical phonon anomaly and unveil a new mode at 0.3 THz that diminishes in amplitude under increasing photocarrier density. Temperature-dependent measurements suggest that the transverse-like modes at 1 and 1.5 THz are possibly of different origins. These results indicate that the unusual phononic properties in PbTe are tunable via photoexcitation and enable new optical functionalities in THz applications, such as spectrally tunable emitters and all-optical modulators.