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Register a new userAb initio calculation of the detailed balance limit to the photovoltaic efficiency of single p-n junction kesterite solar cells
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The thermodynamic limit of photovoltaic efficiency for a single-junction solar cell can be readily predicted using the bandgap of the active light absorbing material. Such an approach overlooks the energy loss due to non-radiative electron-hole processes. We propose a practical ab initio procedure to determine the maximum efficiency of a thin-film solar cell that takes into account both radiative and non-radiative recombination. The required input includes the frequency-dependent optical absorption coefficient, as well as the capture cross-sections and equilibrium populations of point defects. For kesterite-structured Cu$_2$ZnSnS$_4$, the radiative limit is reached for a film thickness of around 2.6 micrometer, where the efficiency gain due to light absorption is counterbalanced by losses due to the increase in recombination current.
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Transition metal dichalcogenide (TMD) materials have emerged as promising candidates for thin film solar cells due to their wide bandgap range across the visible wavelengths, high absorption coefficient and ease of integration with both arbitrary substrates as well as conventional semiconductor technologies. However, reported TMD-based solar cells suffer from relatively low external quantum efficiencies (EQE) and low open circuit voltage due to unoptimized design and device fabrication. This paper studies $Pt/WSe_2$ vertical Schottky junction solar cells with various $WSe_2$ thicknesses in order to find the optimum absorber thickness.Also, we show that the photovoltaic performance can be improved via $Al_2O_3$ passivation which increases the EQE by up to 29.5% at 410 nm wavelength incident light. The overall resulting short circuit current improves through antireflection coating, surface doping, and surface trap passivation effects. Thanks to the ${Al_2O_3}$ coating, this work demonstrates a device with open circuit voltage ($V_{OC}$) of 380 mV and short circuit current density ($J_{SC}$) of 10.7 $mA/cm^2$. Finally, the impact of Schottky barrier height inhomogeneity at the $Pt/WSe_2$ contact is investigated as a source of open circuit voltage lowering in these devices
The intermediate band solar cell (IBSC) and quantum ratchet solar cell (QRSC) have the potential to surpass the efficiency of standard single-junction solar cells by allowing sub-gap photon absorption through states deep inside the band gap. High efficiency IBSC and QRSC devices have not yet been achieved, however, since introducing mid-gap states also increases recombination, which can harm the device. We consider the electronically coupled upconverter (ECUC) solar cell and show that it can achieve the same efficiencies as the QRSC. Although they are equivalent in the detailed balance limit, the ECUC is less sensitive to nonradiative processes, which makes it a more practical implementation for IB devices. We perform a case study of crystalline-silicon based ECUC cells, focusing on hydrogenated amorphous silicon as the upconverter material and highlighting potential dopants for the ECUC. These results illustrate a new path for the development of IB-based devices.
The Shockley-Queisser (SQ) limit provides a convenient metric for predicting light-to-electricity conversion efficiency of a solar cell based on the band gap of the light-absorbing layer. In reality, few materials approach this radiative limit. We develop a formalism and a computational method to predict the maximum photovoltaic efficiency of imperfect crystals from first principles. Our scheme includes equilibrium populations of native defects, their carrier-capture coefficients, and the associated recombination rates. When applied to kesterite solar cells, we reveal an intrinsic limit of 20% for $mathrm{Cu_2ZnSnSe_4}$, which falls far below the SQ limit of 32%. The effects of atomic substitution and extrinsic doping are studied, leading to pathways for enhanced efficiency of 31%. This approach can be applied to support targeted-materials selection for future solar-energy technologies.
Aqueous precursors provide an alluring approach for low-cost and environmentally friendly production of earth-abundant Cu2ZnSn(S,Se)4 (CZTSSe) solar cells. The key is to find an appropriate molecular agent to prepare a stable solution and optimize the coordination structure to facilitate the subsequent crystallization process. Herein, we introduce thioglycolic acid, which possesses strong coordination (-SH) and hydrophilic (-COOH) groups, as the agent and use deprotonation to regulate the coordination competition within the aqueous solution. Ultimately, metal cations are adequately coordinated with thiolate anions, and carboxylate anions are released to become hydrated to form an ultrastable aqueous solution. These factors have contributed to achieving CZTSSe solar cells with efficiency of as high as 12.2% (a certified efficiency of 12.0%) and providing an extremely wide time window for precursor storage and usage. This work represents significant progress in the non-toxic solution fabrication of CZTSSe solar cells and holds great potential for the development of CZTSSe and other metal sulfide solar cells.
Various thin-film I$_2$-II-IV-VI$_4$ photovoltaic absorbers derived from kesterite Cu$_2$ZnSn(S,Se)$_4$ have been synthesized, characterized, and theoretically investigated in the past few years. The availability of this homogeneous materials dataset is an opportunity to examine trends in their defect properties and identify criteria to find new defect-tolerant materials in this vast chemical space. We find that substitutions on the Zn site lead to a smooth decrease in band tailing as the ionic radius of the substituting cation increases. Unfortunately, this substitution strategy does not ensure the suppression of deeper defects and non-radiative recombination. Trends across the full dataset suggest that Gaussian and Urbach band tails in kesterite-inspired semiconductors are two separate phenomena caused by two different antisite defect types. Deep Urbach tails are correlated with the calculated band gap narrowing caused by the (2I$_mathrm{II}$+IV$_mathrm{II}$) defect cluster. Shallow Gaussian tails are correlated with the energy difference between the kesterite and stannite polymorphs, which points to the role of (I$_mathrm{II}$+II$_mathrm{I}$) defect clusters involving Group IB and Group IIB atoms swapping across textit{different} cation planes. This finding can explain why textit{in-plane} cation disorder and band tailing are uncorrelated in kesterites. Our results provide quantitative criteria for discovering new kesterite-inspired photovoltaic materials with low band tailing.
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