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McGott, Deborah L.

Publications and source records attributed to McGott, Deborah L..

Investigation of Sub‐Bandgap Emission and Unexpected n‐Type Behavior in Undoped Polycrystalline CdSe x Te 1‐x

Abstract Se alloying has enabled significantly higher carrier lifetimes and photocurrents in CdTe solar cells, but these benefits can be highly dependent on CdSe x Te 1‐x processing. This work evaluates the optoelectronic, chemical, and electronic properties of thick (3 µm) undoped CdSe x Te 1‐x of uniform composition and varied processing conditions (CdSe x Te 1‐x evaporation rate, CdCl 2 anneal, Se content) chosen to reflect various standard device processing conditions. Sub‐bandgap defect emission is observed, which increased as Se content increased and with “GrV‐optimized CdCl 2 ” (i.e., CdCl 2 anneal conditions used for group‐V‐doped devices). Low carrier lifetime is found for GrV‐optimized CdCl 2 , slow CdSe x Te 1‐x deposition, and low‐Se films. Interestingly, all films (including CdTe control) exhibited n‐type behavior, where electron density increased with Se up to an estimated ≈10 17 cm −3 . This behavior appears to originate during the CdCl 2 anneal, possibly from Se diffusion leading to anion vacancy (e.g., V Se , V Te ) and Cl Te generation.

14 SOLAR ENERGY↗

12.3% Efficient Lifted-Off and Reconstructed As-Doped CdTe Thin Film Solar Cell

CdTe:As devices grown by MOCVD in the superstrate configuration have been reconfigured to a substrate structure, by employing a cleaving and reconstruction technique. Indium and aluminium doped Zinc oxide (IZO and AZO) layers were used as the transparent front interface without a metal grid. A substrate efficiency of 12.3% was realized with AZO front contact, retaining 80% of the superstrate device efficiency and an impressive approximately 99% of the open-circuit voltage. The IZO-based substrate device on the other hand performed at approximately 69 % retained efficiency. The crucial role of front interfaces is highlighted by the two contacts used here. The results in this work show promise for the development of highly efficient substrate CdTe:As devices.

II-VI semiconductor materials↗

Cadmium Telluride Solar Cells: From Fundamental Science to Commercial Applications

In order to meet aggressive decarbonization goals, photovoltacs (PV) need to expand substantially. The current technology that heavily dominates the market, silicon (Si), comprises 95% of the world's PV production, is energy intensive to make, and can take up a substantial portion of the remaining carbon budget if expanded. Conversely, cadmium telluride (CdTe) comprises much of the remaining 5% of the global PV market and has a significantly lower carbon footprint than Si, historically costs less to produce, and is critically important to U.S. competitiveness in the global market. Importantly, CdTe still has room to grow, particularly related to efficiency because voltage has historically been much lower than what we calculate it should be. My research is focused in part on understanding this voltage deficit from a fundamental perspective by studying bulk materials and interfaces. One of the most important regions of the device is buried within the stack, so I developed a technique to cleave and reveal buried interfaces. This cleave technique has enabled a much better scientific understanding and allows us to make lightweight, flexible PV while maintaining low costs, high efficiency, and high throughput associated with standard module processing.

CdTe↗

Thermomechanical Cleave of Polycrystalline CdTe Solar Cells and its Applications: A Review

One of the primary research challenges for cadmium telluride (CdTe) solar cells is addressing its open‐circuit voltage ( V OC ) deficit. While theoretical studies and single crystal work show V OC > 1 V is possible, devices remain stubbornly low at ≈800–900 mV. As absorber opto‐electronic properties (e.g., hole density, carrier lifetime) are improved, device modeling suggests that interfaces become limiting. Because CdTe‐based devices are typically grown in the superstrate configuration, the back interface is relatively accessible for manipulation and study, while the front interface (i.e., the heterojunction region) is buried under microns of material and inaccessible. NREL has developed a novel technique to thermomechanically cleave polycrystalline CdTe device stacks directly at the front interface, enabling characterization and controlled manipulation of this important region. Herein, recent work, primarily from NREL, will be reviewed, including considerations for achieving successful delamination; key scientific discoveries about the front interface that have been enabled by this technique; and practical applications, such as flexible, low‐cost solar with high power‐to‐weight ratio.

14 SOLAR ENERGY↗

Codesigning Alloy Compositions of CdSe y Te 1− y Absorbers and Mg x Zn 1− x O Contacts to Increase Solar Cell Efficiency

Thin‐film solar cells such as CdTe are a major commercial photovoltaic technology, with more than 25 GW installed worldwide and levelized costs of electricity competitive with fossil fuels. Further progress may result from integrating CdSe y Te 1− y absorbers with Mg x Zn 1− x O contacts, but the device efficiency is difficult to maximize due to coupled dependence on chemical composition of both alloys. Herein, a high‐throughput approach is demonstrated to codesign chemical compositions in alloyed Mg x Zn 1− x O/CdSe y Te 1− y thin‐film solar cells, using combinatorial libraries of PV devices with orthogonal composition gradients in CdSe y Te 1− y absorbers and Mg x Zn 1− x O contacts. It is found that the solar cell performance is a strong and coupled function of both elemental compositions, with efficiency up to 17.7% ( V OC = 836 mV, fill factor = 69%, J SC = 30.6 mA cm −2 ) at atomic compositions of Mg/(Mg + Zn) ≈18% and average Se/(Se + Te) ≈4%. These performance trends among >100 devices are explained by >100 ns lifetime of photoexcited charge carriers at the Mg x Zn 1− x O/CdSe y Te 1− y interface where strong Se accumulation is also observed. This study reports the optimal compositions of the commercially relevant Mg x Zn 1− x O/CdSe y Te 1− y solar cells and demonstrates a general approach to codesigning performance of alloyed thin‐film solar cells and other optoelectronic devices.

14 SOLAR ENERGY↗

Evaluation of PbTe and SnTe as Ohmic Contact Layers in CdTe Solar Cell Devices

For solar cells based on CdTe, the choice of a suitable back contact material is limited by CdTe's deep work function. Here, we explored p-type PbTe and SnTe as ohmic contacts to CdTe. These contact layers were grown on single crystal CdTe substrates by molecular beam epitaxy, and the valence band offset between film and substrate was measured using X-ray photoemission spectroscopy. Polycrystalline device structures were also grown by sublimation to assess performance improvements. Doping was achieved in PbTe by thallium incorporation. Only the highest Tl doped PbTe resulted in a desirable band alignment with the CdTe, forming an electron reflector and no hole barrier. Time-resolved photoluminescence measurements also revealed significant photocarrier lifetime improvements for only the highest doped PbTe. Consequentially, devices incorporating the highest doped PbTe layers showed increased power conversion efficiency, primarily from increased fill factor. Doping of the PbTe was measured via Hall effect with variable magnetic field, which was required due to the formation of an n-type parasitic interface layer. To properly interpret the variable field Hall measurements, we derived an expression for the magnetic field-dependent conductivity tensor of an L-valley semiconductor.

anisotropic band valley↗

Epitaxial Dirac Semimetal Vertical Heterostructures for Advanced Device Architectures

Exploiting the extraordinary transport and optical properties of 3D topological semimetals for device applications requires epitaxial integration with semiconductors to carefully control carrier transport, yet no studies have established heteroepitaxy on top of any topological semimetals to date. Here, a novel approach toward fabricating heterostructures is demonstrated by epitaxially incorporating the Dirac semimetal Cd 3 As 2 between Zn x Cd 1-x Te and CdTe layers via molecular beam epitaxy on GaAs (001) substrates. The approach utilizes the higher energy (001) surface of Cd 3 As 2 to stabilize 2D epitaxy of zinc blende semiconductors. To demonstrate the impact heterostructure formation offers to device performance, an all-epitaxial, barrier-type vertical photodetector is fabricated that accesses a different carrier separation mechanism than previously reported non-epitaxial junctions and consequently exhibits significantly reduced dark currents. Finally, the results highlight the important role that epitaxial integration can play in accessing advanced architectures for topological semimetal-based devices.

36 MATERIALS SCIENCE↗

Dual-Wavelength Time-Resolved Photoluminescence Study of CdSe x Te 1-x Surface Passivation via Mg y Zn 1-y O and Al 2 O 3

Voltage loss is currently one of the biggest challenges facing cadmium telluride (CdTe) based photovoltaics. Determining the location(s) of major voltage loss within the device stack (e.g., front/back interface, grain boundaries) is therefore of primary interest. Here, we present a custom-built time-resolved photoluminescence system with two excitation wavelengths - 670 (standard) and 405 nm - to probe the device stack at depths of approximately 130 and 35 nm, respectively; their comparison helps differentiate interface and bulk contributions to carrier lifetime. We apply this system to examine the passivation effect of two significant recent advances in CdTe: the incorporation of Se to form graded CdSe x Te 1-x and the replacement of CdS with Mg y Zn 1-y O. It is found that x = 0.2 Se is required to obtain lifetime improvements, primarily in the bulk. Additionally, evidence for trapping at the Mg y Zn 1-y O/CdSe x Te 1-x interface was observed. Furthermore, this indicates further work is required to sufficiently passivate the front interface.

CdSeTe↗

Carrier Lifetime as a Function of Se Content for CdSexTe1-x Films Grown on Al2O3 and MgZnO: Preprint

Time-resolved photoluminescence (TRPL) with two excitation wavelengths – 670 (standard) and 405 nm – was used to examine the effect on carrier lifetime of two significant recent advances in CdTe: the incorporation of Se to form graded CdSe x Te 1-x and the use of Mg y Zn 1-y O buffers. The two excitation wavelengths probe depths of approximately 130 and 35 nm, respectively, and their comparison helps differentiate interface and bulk contributions to carrier lifetime. It was found that x = 0.2 Se was required to obtain lifetime improvements, primarily in the bulk. Additionally, TRPL traces for Mg y Zn 1-y O/CdSe x Te 1-x samples showed fast initial decay followed by a long-lived tail, which may be indicative of trap-dominated recombination. This behavior was not present for CdSe x Te 1-x films grown on Al 2 O 3 , which is currently state-of-the-art for surface passivation in CdTe. This indicates that further work is required to sufficiently passivate the front interface.

cadmium telluride↗

Carrier Lifetime as a Function of Se Content for CdSexTe1-x Films Grown on Al2O3 and MgZnO

Time-resolved photoluminescence (TRPL) with two excitation wavelengths – 670 (standard) and 405 nm – was used to examine the effect on carrier lifetime of two significant recent advances in CdTe: the incorporation of Se to form graded CdSe x Te 1-x and the use of Mg y Zn 1-y O buffers. The two excitation wavelengths probe depths of approximately 130 and 35 nm, respectively, and their comparison helps differentiate interface and bulk contributions to carrier lifetime. It was found that x = 0.2 Se was required to obtain lifetime improvements, primarily in the bulk. Additionally, TRPL traces for Mg y Zn 1-y O/CdSe x Te 1-x samples showed fast initial decay followed by a long-lived tail, which may be indicative of trap-dominated recombination. This behavior was not present for CdSe x Te 1-x films grown on Al 2 O 3 , which is currently state-of-the-art for surface passivation in CdTe. This indicates that further work is required to sufficiently passivate the front interface.

cadmium telluride↗

Is 3D/2D Passivation a Secret to Success for Polycrystalline Thin-Film Solar Cells?

Three leading thin-film photovoltaic (PV) technologies - cadmium telluride (CdTe), CuIn1-xGaxSe2 (CIGS), and perovskite solar cells (PSCs) - are all polycrystalline, but otherwise appear to have little in common. A comprehensive examination of these technologies, however, reveals a common theme: the formation of two-dimensional (2D) van der Waals materials at three-dimensional (3D) absorber interfaces and grain boundaries. In CdTe, the 2D compound is CdCl2; in CIGS, it is XInSe2 (X= K, Rb, Cs) with X depending on the heavy-alkali post-deposition treatment used; and in lead halide PSCs, PbI2 forms naturally, but many new, more stable, 2D perovskites have also been incorporated. Generally, these 2D interfacial materials are present not by design, but instead have evolved from their 3D counterparts during standard device processing. Here, new data, together with evidence compiled from the literature, are presented to illustrate both the existence of 3D/2D interfaces in CdTe, CIGS, and PSCs, and their correlation with improved passivation and device performance. This suggests that 3D/2D passivation may be a heretofore unappreciated key to successful polycrystalline thin-film PV. Finally, the desired attributes of successful low-dimensional layers are presented with rational design strategies for next generation polycrystalline solar cells.

3D/2D↗

Emitter Reconstruction for Cleaved CdSexTe1-x Devices with Cu vs. As Doping

CdTe absorbers have had historically low carrier densities of ~10^14 cm-3 due to the self-compensating nature of copper dopants. Recent advances in group-V (e.g., arsenic) doping have increased this to 10^16-10^17 cm-3, but modeling suggests that the front interface and emitter properties become limiting in this case. By cleaving arsenic- and copper-doped CdTe device stacks at the emitter/absorber interface, we gain the ability to reconstruct emitters with known properties, which will not change during subsequent device processing, and directly test the modeling. By doing so, we find a much larger performance drop in arsenic devices; this is attributed to insufficient electron density in the emitter and increased sensitivity to interface changes due to collapsed depletion width. This work can help guide emitter engineering for highly-doped CdTe devices in both the as-grown-superstrate- and cleaved-substrate configurations.

As-doped↗

Development of arsenic doped Cd(Se,Te) absorbers by MOCVD for thin film solar cells

Recent developments in CdTe solar cell technology have included the incorporation of ternary alloy Cd(Se,Te) in the devices. CdTe absorber band gap grading due to Se alloying contributes to current density enhancement and can result in device performance improvement. Here we report Cd(Se,Te) polycrystalline thin films grown by a chamberless inline atmospheric pressure metal organic chemical vapour deposition technique, with subsequent incorporation in CdTe solar cells. The compositional dependence of the crystal structure and optical properties of Cd(Se,Te) are examined. Selenium graded Cd(Se,Te)/CdTe absorber structure in devices are demonstrated using either a single CdSe layer or CdSe/Cd(Se,Te) bilayer (with or without As doping in the Cd(Se,Te) layer). Cross-sectional TEM/EDS, photoluminescence spectra and secondary ion mass spectroscopy analysis confirmed the formation of a graded Se profile toward the back contact with a diffusion length of ~1.5 um and revealed back-diffusion of Group V (As) dopants from the CdTe layer into Cd(Se,Te) grains. Due to the strong Se/Te interdiffusion, CdSe in the Se bilayer configuration was unable to form an n-type emitter layer in processed devices. In situ As doping of the Cd(Se,Te) layer benefited the device junction quality with current density reaching 28.3 mA/cm 2 . The results provide useful insights for the optimisation of Cd(Se,Te)/CdTe solar cells.

14 SOLAR ENERGY↗