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At least 415 records · Page 23

Stacking polymorphism of PtSe 2 : its implication to layer-dependent metal-insulator transitions

Using diffusion Monte Carlo (DMC) and density functional theory (DFT) calculations, we examine the structural stability and interlayer binding properties of PtSe 2 . Our DMC study reveals that AA and AB-r bilayer stacking modes are nearly degenerate, highlighting the significant role of interlayer hybridization in offsetting the energy cost due to larger interlayer separations in the AB-r mode. Additionally, our DMC-benchmarked DFT calculations with the r 2 SCAN+rVV10 functional uncover pronounced stacking polymorphism in few-layer PtSe 2 , driven by degenerate AA and AB-r interfaces, which leads to substantial band gap variations across different stacking configurations. This polymorphism, along with selenium vacancies, influences a layer-dependent metal-insulator transition observed in few-layer PtSe 2 . Our findings emphasize the importance of both van der Waals interactions and interlayer hybridization in determining the phase stability and electronic properties of PtSe 2 , advancing our understanding of its fundamental properties and refining theoretical models for practical applications in nanoelectronic devices.

Electronic materials↗

Comparison of Fission Product Release Predictions using PARFUME and BISON with Results from the AGR-3/4 Irradiation Experiment

The PARFUME (PARticle Fuel ModEl) fuel performance modeling code and the BISON nuclear fuel performance application built on the Multiphysics Object-Oriented Simulation Environment (MOOSE) finite element library were used to predict the fission product release from tristructural isotropic (TRISO) coated fuel particles and compacts during the third and fourth irradiation experiment of the Advanced Gas Reactor (AGR-3/4) Fuel Development and Qualification Program. The fuel performance modeling codes PARFUME and BISON modeled the AGR-3/4 irradiation experiment using the fuel compact time-averaged volume averaged (TAVA) daily temperatures for a total irradiation duration of 369.1 effective full power days (EFPD) to predict the release fraction of the fission product silver (Ag-110m) from a representative TRISO-coated fuel particle from AGR-3/4 compacts. Post-irradiation examination (PIE) measurements provided data on the release of these fission products in the compacts outside of the silicon carbide (SIC) layer. The PARFUME and BISON results were then compared to the silver release measured from compact gamma scanning. The results showed good agreement between PARFUME and BISON but both codes under-predicted the silver release fraction for all the compacts. In addition, BISON was used to model and predict the fission product concentration radial profile outside of the compacts in capsules’ inner and outer rings. These rings were either comprised of matrix and/or structural graphite. To obtain the concentration profiles of silver, cesium, and strontium, a sorption isotherm model was developed in BISON to capture the effects of fission product transport across the gaps between the concentric rings. The general shape of the concentration radial profiles as calculated by BISON were similar in the inner ring (IR) but varied in the outer ring (OR) depending on the fission product of interest or capsule temperature. Using this methodology and model, BISON now has the capability to aid in developing new fission product diffusion coefficients for matrix or structural graphite materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Electro-Optical Characterization of Arsenic-Doped CdSeTe and CdTe Solar Cell Absorbers Doped in-situ During Close Space Sublimation

Most contemporary device models predict that an acceptor concentration of at least 10^16 cm^-3 is required to reach an open circuit voltage of 1 V in polycrystalline CdTe-based solar cells. While copper has traditionally been used as the de facto p-type dopant in polycrystalline cadmium telluride (CdTe) and cadmium selenide telluride (CdSeTe), reaching high acceptor concentrations has proved to be challenging in such devices due to significant dopant compensation. The acceptor concentration in copper-doped CdTe and CdSeTe typically ranges from 10^13 to 10^15 cm^-3 and routinely exhibit low external radiative efficiencies below 0.01%, limiting their implied voltage (i.e., quasi-Fermi level splitting) to approximately 900 mV. As an alternative to copper, this work explores the use of arsenic as a p-type dopant for CdTe and CdSeTe. Using a novel technique in which a thin layer of arsenic-containing material is deposited and used as a reservoir for arsenic to diffuse into a front layer of previously undoped material, this contribution demonstrates that high external radiative efficiencies are achievable, a direct result of combined high acceptor concentrations and long minority-carrier lifetimes in the absorber. This leads to improved implied voltages, and indicates that As-doping represents a promising pathway towards improving the external voltage of CdSeTe/CdTe solar cells.

cadmium telluride↗

Dynamics of Electric Polarization and Relaxation of Ions at Humid Calcite Surfaces

Mobile ions at mineral surfaces can respond to an applied electric field, adopting a new distribution that effectively represents polarization of the electrical double layer. When the field is released, the ions relax to their equilibrium distribution. In both cases, the dynamics are characteristic of the interface. However, current models of electrokinetic phenomena are not sufficiently robust to accurately predict collective ion dynamics at structurally and chemically specific mineral–water interfaces. Here, in this study, we use electrostatic force microscopy (EFM) to investigate the dynamics of ion relaxation at hydrated calcite (104) surfaces at controlled relative humidity (RH). Electrically biased probes are used to polarize the distributions of calcium and carbonate ions that are intrinsic to this interface across a range of RH values. Polarization kinetics are tracked by monitoring the tip–sample force gradient during charging, and EFM imaging is used to characterize the spatial relaxation dynamics after the applied field is released. Electrostatic finite element modeling of the sample/probe system across length-scales from nanometers to millimeters reproduces the observed stretched exponential charging response. Together, these results allow us to estimate the ion diffusivities at the interface across a wide range of RH values. These diffusivities increase by roughly 5 orders of magnitude as the RH is increased from 5 to 90%, highlighting the critical role of adsorbed water for surface ion solvation that enables ion mobility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Computational general relativistic force-free electrodynamics: II. Characterization of numerical diffusivity

Scientific codes are an indispensable link between theory and experiment; in (astro-)plasma physics, such numerical tools are one window into the universe’s most extreme flows of energy. The discretization of Maxwell’s equations – needed to make highly magnetized (astro)physical plasma amenable to its numerical modeling – introduces numerical diffusion. It acts as a source of dissipation independent of the system’s physical constituents. Understanding the numerical diffusion of scientific codes is the key to classifying their reliability. It gives specific limits in which the results of numerical experiments are physical. We aim at quantifying and characterizing the numerical diffusion properties of our recently developed numerical tool for the simulation of general relativistic force-free electrodynamics by calibrating and comparing it with other strategies found in the literature. Our code correctly models smooth waves of highly magnetized plasma. We evaluate the limits of general relativistic force-free electrodynamics in the context of current sheets and tearing mode instabilities. We identify that the current parallel to the magnetic field (j ∥ ), in combination with the breakdown of general relativistic force-free electrodynamics across current sheets, impairs the physical modeling of resistive instabilities. We find that at least eight numerical cells per characteristic size of interest (e.g., the wavelength in plasma waves or the transverse width of a current sheet) are needed to find consistency between resistivity of numerical and of physical origins. High-order discretization of the force-free current allows us to provide almost ideal orders of convergence for (smooth) plasma wave dynamics. The physical modeling of resistive layers requires suitable current prescriptions or a sub-grid modeling for the evolution of j ∥ .

79 ASTRONOMY AND ASTROPHYSICS↗

Defect characterization and charge transport measurements in high-resolution Ni/n-4H-SiC Schottky barrier radiation detectors fabricated on 250 μ m epitaxial layers

Advances in the growth processes of 4H-SiC epitaxial layers have led to the continued expansion of epilayer thickness, allowing for the detection of more penetrative radioactive particles. In this work, we report the fabrication and characterization of high-resolution Schottky barrier radiation detectors on 250 μm thick n-type 4H-SiC epitaxial layers, the highest reported thickness to date. Several 8 × 8 mm 2 detectors were fabricated from a diced 100 mm diameter 4H-SiC epitaxial wafer grown on a conductive 4H-SiC substrate with a mean micropipe density of 0.11 cm -2 From the Mott–Schottky plots, the effective doping concentration was found to be in the range (0.95–1.85) × 10 14 cm -3 , implying that full depletion could be achieved at ~5.7 kV (0.5 MV/cm at the interface). The current-voltage characteristics demonstrated consistently low leakage current densities of 1–3 nA/cm 2 at a reverse bias of -800 V. This resulted in the pulse-height spectra generated using a 241Am alpha source (5486 keV) manifesting an energy resolution of less than 0.5% full width at half maximum (FWHM) for all the detectors at -200 V. The charge collection efficiencies (CCEs) were measured to be 98–99% with no discernable correlation to the energy resolution. A drift-diffusion model fit to the variation of CCE as a function of bias voltage, revealed a minority carrier diffusion length of ~10 μm. Deep level transient spectroscopy measurements on the best resolution detector revealed that the excellent performance was the result of having ultralow concentrations of the order of 1011 cm-3 lifetime limiting defects—Z 1/2 and EH 6/7 .

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Evaluating alternative ebullition models for predicting peatland methane emission and its pathways via data–model fusion

Abstract. Understanding the dynamics of peatland methane (CH4) emissions and quantifying sources of uncertainty in estimating peatland CH4 emissions are critical for mitigating climate change. The relative contributions of CH4 emission pathways through ebullition, plant-mediated transport, and diffusion, together with their different transport rates and vulnerability to oxidation, determine the quantity of CH4 to be oxidized before leaving the soil. Notwithstanding their importance, the relative contributions of the emission pathways are highly uncertain. In particular, the ebullition process is more uncertain and can lead to large uncertainties in modeled CH4 emissions. To improve model simulations of CH4 emission and its pathways, we evaluated two model structures: (1) the ebullition bubble growth volume threshold approach (EBG) and (2) the modified ebullition concentration threshold approach (ECT) using CH4 flux and concentration data collected in a peatland in northern Minnesota, USA. When model parameters were constrained using observed CH4 fluxes, the CH4 emissions simulated by the EBG approach (RMSE = 0.53) had a better agreement with observations than the ECT approach (RMSE = 0.61). Further, the EBG approach simulated a smaller contribution from ebullition but more frequent ebullition events than the ECT approach. The EBG approach yielded greatly improved simulations of pore water CH4 concentrations, especially in the deep soil layers, compared to the ECT approach. When constraining the EBG model with both CH4 flux and concentration data in model–data fusion, uncertainty of the modeled CH4 concentration profiles was reduced by 78 % to 86 % in comparison to constraints based on CH4 flux data alone. The improved model capability was attributed to the well-constrained parameters regulating the CH4 production and emission pathways. Our results suggest that the EBG modeling approach better characterizes CH4 emission and underlying mechanisms. Moreover, to achieve the best model results both CH4 flux and concentration data are required to constrain model parameterization.

59 BASIC BIOLOGICAL SCIENCES↗

Incorporating Electrochemical Halide Oxidation into Drift-Diffusion Models to Explain Performance Losses in Perovskite Solar Cells under Prolonged Reverse Bias

Partial shading of a solar module can induce a set of cells within the module to operate under reverse bias. Studies have shown that metal halide perovskite solar cells with a wide variety of compositions and contacts exhibit interesting behavior in reverse bias that includes both reversible performance loss and non-reversible degradation. In this paper, an advanced drift-diffusion approach incorporating an electrochemical term to explain the short-circuit, open circuit and fill factor losses that are experimentally measured after prolonged reverse bias is used. It is shown that holes can tunnel into the perovskite due to sharp band bending near the contact, accumulate within the bulk of the perovskite absorber, and trigger the oxidation of halides to form neutral halogens. The density of neutral halogens is much higher in reverse bias because there are hardly any electrons available to reduce the iodine. The resulting halogens act as bulk recombination centers. While the interstitial halogen density does decay when the cell is operated in forward bias, permanent degradation can occur if the iodine diffuses out of the perovskite layer. Finally, the ways in which changing parameters such as the mobile ion density or the series resistance at the contact can influence device performance and stability are discussed.

degradation↗

Generation of mean flows in rotating anisotropic turbulence: The case of solar near-surface shear layer

Results from helioseismology indicate that the radial gradient of the rotation rate in the near-surface shear layer (NSSL) of the Sun is independent of latitude and radius. Theoretical models using the mean-field approach have been successful in explaining this property of the NSSL, while global direct or large-eddy magnetoconvection models have so far been unable to reproduce this. We investigate the reason for this discrepancy by measuring the mean flows, Reynolds stress, and turbulent transport coefficients under conditions mimicking those in the solar NSSL. Simulations with as few ingredients as possible to generate mean flows were studied. These ingredients are inhomogeneity due to boundaries, anisotropic turbulence, and rotation. The parameters of the simulations were chosen such that they matched the weakly rotationally constrained NSSL. The simulations probe locally Cartesian patches of the star at a given depth and latitude. The depth of the patch was varied by changing the rotation rate such that the resulting Coriolis numbers covered the same range as in the NSSL. We measured the turbulent transport coefficient relevant for the nondiffusive (Λ-effect) and diffusive (turbulent viscosity) parts of the Reynolds stress and compared them with predictions of current mean-field theories. A negative radial gradient of the mean flow is generated only at the equator where meridional flows are absent. At other latitudes, the meridional flow is comparable to the mean flow corresponding to differential rotation. We also find that the meridional components of the Reynolds stress cannot be ignored. Additionally, we find that the turbulent viscosity is quenched by rotation by about 50% from the surface to the bottom of the NSSL. Our local simulations do not validate the explanation for the generation of the NSSL from mean-field theory where meridional flows and stresses are neglected. However, the rotational dependence of the turbulent viscosity in our simulations agrees well with theoretical predictions. Moreover, our results agree qualitatively with global convection simulations in that an NSSL can only be obtained near the equator.

79 ASTRONOMY AND ASTROPHYSICS↗

Understanding the TiH (2-x) /TiO y System at Elevated Temperature: A Literature Review

Titanium hydride of varying TiH stoichiometry is used in pyrotechnic compositions. In order to yield consistent performance, manufacturing processes must be developed to ensure precise and reproducible material properties, including composition and morphology. Legacy synthesis protocols are not comprehensive nor are the required apparatuses still available. To guide the development of novel production procedures, this report reviews literature on relevant chemical reactions and diffusion events occurring at elevated temperature in the TiH (2-x) /TiO y system. Titanium hydride exposed to air spontaneously forms a passivating oxide layer. Upon heating, significant hydrogen release, which is accompanied by changes to the surface oxide layer, is noted by 375–400°C. At higher temperatures (above about 500°C) the oxide layer is reported to be essentially nonexistent as a result of oxide-layer dissolution processes and, potentially, oxide-layer reduction due to water formation. Based on the reviewed literature, we hypothesize that, by 500°C, the surface layer consists of an oxyhydride phase, which is a solid solution of oxygen in titanium hydride. We believe that hydrogen release from titanium hydride is controlled by the kinetics of molecular hydrogen desorption on the oxyhydride surface. No literature data is available for corresponding activation energies of the dynamic desorption process, and the equilibrium phase diagram of this three-component system remains largely unexplored as well. These gaps in knowledge might be addressed through coordinated computational modeling and experimental efforts.

36 MATERIALS SCIENCE↗

Cadmium Selective Etching in CdTe Solar Cells Produces Detrimental Narrow-Gap Te in Grain Boundaries

Recent advances in design and processing technology have made possible commercialization of polycrystalline (px)-CdTe as a photovoltaic absorber. Grain boundaries (GBs) are the most prominent structural defects in these devices and undergo significant changes during device fabrication. However, the effects of device fabrication processes on these GBs are not entirely understood. Prevailing models of GBs in thin-film photovoltaics consider individual GBs to have homogeneous properties in their area. Here, using an aberration-corrected scanning transmission electron microscope (STEM)-based low-loss and core-loss electron energy-loss spectroscopy (EELS), we show that back-surface etching of CdTe leads to inhomogeneity within individual grain boundaries. We observe that etching the back surface leads to the conversion of a region of GBs from CdTe to an elemental Te, which has an only 0.33 eV band gap, as deep as 1 μm from the back surface. The presence of elemental Te in GBs this deep into the absorber layer will increase recombination in the absorber layer and limit the extractable open-circuit voltage, thus reducing device efficiency. However, additive methods for back contact formation such as deposition of Te, ZnTe, or other materials preserve the CdTe stoichiometry of the GBs. Thus, especially for the next generations of CdTe-based cells having longer minority carrier diffusion length and/or thinner absorber layers, additive back contacting methods are superior.

36 MATERIALS SCIENCE↗

Conservation laws and effective hadronization models

Hadronization models based on local string-breaking dynamics are typically Markovian by construction, yet the physical ensemble of final states is shaped by global constraints that couple the entire fragmentation trajectory. Recasting hadronization as a conditioned stochastic diffusion process provides a precise mathematical resolution to this tension. In particular, this language reveals explicitly that constraints stemming from conservation laws induce non-Markovian correlations between otherwise independent fragmentation steps, and that these correlations can be absorbed exactly into a renormalization of the local dynamics through a Doob $h$-transform. We develop this formalism for a $q\bar{q}$ string in the chiral limit, where the longitudinal-transverse factorization of the Lund kernel becomes exact, enabling systematic power counting and clean ultraviolet (UV)/infrared (IR) separation. The dynamics organize naturally into a tower of effective theories distinguished by the remaining string mass, spanning a UV fixed point with scale-invariant transport coefficients, an intermediate regime where transverse phase space induces controlled running, and an IR boundary layer where non-local effects enter at leading order. The tower exhibits genuine Wilsonian structure, including $β$-functions, anomalous dimensions, and systematic matching conditions. The resulting framework achieves a clean factorization of universal microscopic fragmentation dynamics from infrared constraint effects, and opens new directions for both the theoretical analysis and practical simulation of hadronization.

Menzo, Tony [Alabama U.; Fermilab] (ORCID:00000002↗

MMMnet: A Neural Network Surrogate for Real-Time Transport Prediction Based on the Updated Multi-Mode Model

The Multi-Mode Model (MMM) is a physics-based anomalous transport model integrated into TRANSP for predicting electron and ion thermal transport, electron and impurity particle transport, and toroidal and poloidal momentum transport. While MMM provides valuable predictive capabilities, its computational cost, although manageable for standard simulations, is too high for real-time control applications. MMMnet, a neural network-based surrogate model, is developed to address this challenge by significantly reducing computation time while maintaining high accuracy. Trained on TRANSP simulations of DIII-D discharges, MMMnet incorporates an updated version of MMM (9.0.10) with enhanced physics, including isotopic effects, plasma shaping via effective magnetic shear, unified correlation lengths for ion-scale modes, and a new physics-based model for the electromagnetic electron temperature gradient mode. A key advancement is MMMnet’s ability to predict all six transport coefficients, providing a comprehensive representation of plasma transport dynamics. MMMnet achieves a two-order-of-magnitude speed improvement while maintaining strong correlation with MMM diffusivities, making it well-suited for real-time tokamak control and scenario optimization.

DIII-D↗

Pore-Scale Transport Effects in Electrochemical CO 2 Reduction on Gold via Coupled Microkinetic-Transport Modeling

A pore-resolved modeling framework is developed to quantify how pore-scale transport affects the intrinsic microkinetics of CO 2 -to-CO on Au. A DFT-informed microkinetic model is coupled self-consistently to a Generalized-Modified Poisson–Nernst–Planck (GMPNP) transport description in a single, electrolyte-filled cylindrical pore, allowing local concentrations and potential to feed back into site-specific reaction rates. FIB-SEM is used to determine pore sizes within realistic electrode materials. Across pore diameters, d p = 10–6000 nm, the surface-averaged CO 2 reduction rate is systematically reduced relative to the ideal microkinetic baseline where mass transport is not accounted for; the effectiveness factor 𝜂 𝑠,CO 2 , which quantifies this ratio, decreases rapidly at more negative potentials and is about 1% near −1.0 V vs SHE due to reactant depletion. Spatial maps reveal pore-bulk alkalization that emerges at higher cathodic bias, with a small, near-wall pH dip due to electrostatic repulsion of hydroxide at the cathode interface. For a fixed aspect ratio L p /d p , narrower pores exhibit larger 𝜂 𝑠,CO 2 by shortening diffusion paths, whereas variations in the aspect ratio L p /d p play a secondary role. A dimensionless analysis (surface/bulk Damköhler numbers) delineates operating regimes. In conclusion, this work offers a concept for incorporating microkinetic models into homogenized porous-electrode models through effectiveness factors and pore-size distribution.

Au-catalyst↗

Elevated temperature mechanical properties of Inconel 617 surface oxide using nanoindentation

Inconel 617 is a principal candidate material for helium gas cooled very-high-temperature reactors with outlet temperatures of 700–950 °C. Recent findings showed that this alloy develops unique surface oxide layers especially at high temperature (HT) helium environment with distinctive wear, friction and contact properties. This study investigates the elevated temperature mechanical properties of Inconel 617 top surface layers aged in HT helium environment. Nanoindentation technique is used to obtain load-displacement graphs of the alloy top surface oxide in temperatures ranging from 25 °C up to 600 °C. In addition, using finite element analysis along with an iterative regression technique, a semi-numerical method is developed to further measure and quantify the material parameters and, in particular, time-independent and creep characteristics of the oxide. Although Young's modulus of the oxide is found to be relatively close to the bulk for the tested temperatures, the yield strength and hardness, in comparison to the bulk material, increase significantly as the material is oxidized after aging. The oxide exhibits significant softening as the temperature increases to 600 °C. Unlike the bulk material, diffusion through the grains is found to be the dominant creep mechanism for the oxide. Considerable difference between the mechanical properties of the oxide and the bulk material shows the need for accurate measurements of near surface mechanical properties, if reliable predictive contact and tribological models are sought at elevated temperatures.

36 MATERIALS SCIENCE↗

Diagnosing Near-Surface Model Errors with Candidate Physics Parameterization Schemes for the Multiphysics Rapid Refresh Forecast System (RRFS) Ensemble during Winter over the Northeastern United States and Southern Great Plains

Abstract During the winter of 2020/21 an ensemble of FV3-LAM forecasts was produced over the contiguous United States for the Winter Weather Experiment using five physics suites. These forecasts are evaluated with the goal of optimizing physics parameterizations within the future operational Rapid Refresh Forecast System (RRFS) in the Unified Forecast System (UFS) realm and for selecting suitable physics suites for a multiphysics RRFS ensemble. The five physics suites have different combinations of land surface models (LSMs), planetary boundary layer (PBL) parameterizations, and surface layer schemes, chosen from those used in current and possible future operational systems and likely to be supported in the operational UFS. Full-season evaluation reveals a persistent near-surface cold bias in the U.S. Northeast from one suite and a nighttime warm bias in the southern Great Plains in another suite, while other suites have smaller biases. A representative case is chosen to diagnose the cause for each of these biases using sensitivity simulations with different physics combinations or modified parameters and verified with additional mesonet observations. The cold bias in the Northeast is attributed to aspects of the Noah-MP LSM over snow cover, where Noah-MP simulates lower soil water content, and thus lower thermal conductivity than other LSMs, leading to less upward ground heat flux during nighttime and consequently lower surface temperature. The nighttime warm bias found in the southern Great Plains is attributed to overestimation of vertical mixing in the K -profile-based eddy-diffusivity mass-flux (K-EDMF) PBL scheme and insufficient land–atmospheric coupling from the GFS surface layer scheme over short vegetation. A few key parameters driving these systematic biases are identified.

Meteorology & Atmospheric Sciences↗

Novel Poly-Si:Ga/SiOx Passivating Contacts through Non-Equilibrium Doping

Poly-Si/SiOx passivating contacts are one of the key enablers for high-efficiency, low-cost c-Si solar cells. In recent years, record devices have reached efficiencies of 26% in the laboratory and 25% in the industry. The current cell structure utilizing a tunneling oxide passivating contact structure with a back phosphorus-doped poly- Si/SiOx passivating contact and a front boron diffused emitter suffers from large emitter recombination. Thus, replacing the front B diffused emitter with a p-type passivating contact is a route to overcome this deficiency. This gives rise to front/back poly-Si based passivating contacts. To address the low passivation performance of the B-doped poly-Si passivating contacts, we replace B with Ga as a novel p-type dopant to avoid dopant accumulation in the tunneling oxide, which is known to lead to large degradation loss in passivation quality. Here, we introduce a non-equilibrium method via pulsed laser melting to thermally melt and recrystallize the poly-Si and redistribute the dopants, achieving doping concentrations above the solid solubility limit (~4E19 cm-3). We demonstrate a good passivation quality with an iVoc of 721 mV with an active Ga doping concentration in poly-Si >1020 cm-3. Furthermore, we show a low contact resistivity of 33.2 +/- 9.3 mO cm2 using a diode model calculation. Finally, cross-section scanning spreading resistance microscopy was performed to determine the resistance profile across the non-homogeneously doped poly-Si layer.

c-Si↗