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中国物理学会期刊

载流子输运下钙钛矿电池的能量转换与损耗机制研究

Energy conversion and loss mechanisms of perovskite solar cells based on carrier transport

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  • 本文建立了立方相MAPbI3钙钛矿太阳能电池的光电耦合数值模型。光学上,采用传输矩阵法求解多层薄膜干涉,获得光谱分辨的局域吸收功率密度与光生载流子产生率;电学上,在耦合辐射与非辐射复合损耗机制的基础上,自洽求解泊松方程、漂移扩散方程及连续性方程。在等温框架下,量化热化热、焦耳热及复合热等各损耗,进而评估了不同工作温度下器件的电学输出与能量损耗分配。模拟结果表明,光生载流子产生率由吸收系数与光场协同调控。短波光受寄生吸收与浅穿透所限集中于入射面,长波光因本征吸收弱而产生率降低。电子与空穴浓度同具波长依赖,但能带偏移造成不对称。电子于电子传输层/钙钛矿界面快速提取而骤降,空穴则受价带势垒阻挡而耗尽,于空穴传输层界面富集提取。与文献报道相比,本器件因未考虑离子迁移,光生电流与开路电压更高;但文献中采用ZnO/NiOx的器件,低电压下载流子提取更优,因而电流密度高于本文TiO2/Spiro-OMeTAD组合;该优势随电压升高而减弱,二者在开路电压附近趋同。在最大功率点处,22.4%的太阳能转换为电能,其余78.4%被耗散。其中光学损失与珀尔帖热合计占58.5%,热化损失占7.9%,非辐射表面复合损失占5.6%。温度升高时,热化与焦耳热降低,寄生吸收基本不变,体相与表面复合显著增加,导致输出功率下降。协同光学、能带及界面工程抑制多重损耗,是提升器件性能的有效途径。本研究为钙钛矿太阳能电池性能优化提供了理论依据。

     

    This work develops an optical-electrical coupled numerical model to simulate cubic MAPbI3based perovskite solar cells (PSCs). Optically, the transfer matrix method resolves multilayer interference effects to obtain the spectrally resolved local absorbed power density and photo-generation rate. Electrically, the Poisson, drift-diffusion, and continuity equations are solved self-consistently, incorporating Shockley-Read-Hall, radiative, Auger, and interfacial recombination. On this basis, the power densities of individual loss channels, including thermalization, Joule, and recombination heat, are quantified within an isothermal framework, enabling a systematic evaluation of the device’s electrical output and energy loss allocation under different operating temperatures. The simulation results reveal that the photo-generation rate is governed by the absorption coefficient and local optical field, with the optimal response centered at 460 nm. Short-wavelength light (<400 nm) is confined near the incident surface due to parasitic absorption and shallow penetration, whereas long-wavelength light (>600 nm) suffers from reduced generation owing to weak intrinsic absorption. Electron and hole concentrations follow the same wavelength dependence, but band offsets introduce asymmetry. Electrons are rapidly extracted at the electron transport layer/perovskite absorber layer interface, causing a sharp concentration drop, whereas holes are depleted at the same interface by the electron transport layer valence band barrier and accumulate at the hole transport layer interface for efficient extraction. Compared with literature reports, the present device yields higher photo-generated current and open-circuit voltage because ion migration is excluded, whereas the literature device using ZnO/NiOx transport layers, with their wide band-gaps and suitable band alignment, exhibits more efficient carrier extraction and lower contact resistance at low voltages, thus delivering a higher current density than the TiO2/Spiro-OMeTAD combination adopted in this study. This advantage diminishes at higher voltages as the built-in field weakens, and both current densities converge near open-circuit voltage where recombination dominates. A peak efficiency of 22.4% at the maximum power point is achieved. Of the total incident energy, 78.4% is dissipated as losses, of which optical escape losses and Peltier heat together account for 58.5%, thermalization losses for 7.9%, and non-radiative surface recombination losses for 5.6%. Rising temperature reduces thermalization and Joule losses, leaves parasitic absorption nearly unchanged, but significantly increases bulk and surface recombination, leading to output power degradation. Thus, a synergistic approach combining optical, band, and interface engineering to suppress multiple loss channels offers a promising path for performance enhancement. This study provides a theoretical foundation for loss mitigation and optimization in PSCs.

     

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