Stacking solar cells with decreasing band gaps to form tandems presents the possibility of overcoming the single-junction Shockley-Queisser limit in photovoltaics. The rapid development of solution-processed perovskites has brought perovskite single-junction efficiencies >20%. However, this process has yet to enable monolithic integration with industry-relevant textured crystalline silicon solar cells. We report tandems that combine solution-processed micrometer-thick perovskite top cells with fully textured silicon heterojunction bottom cells. To overcome the charge-collection challenges in micrometer-thick perovskites, we enhanced threefold the depletion width at the bases of silicon pyramids. Moreover, by anchoring a self-limiting passivant (1-butanethiol) on the perovskite surfaces, we enhanced the diffusion length and further suppressed phase segregation. These combined enhancements enabled an independently certified power conversion efficiency of 25.7% for perovskite-silicon tandem solar cells. These devices exhibited negligible performance loss after a 400-hour thermal stability test at 85°C and also after 400 hours under maximum power point tracking at 40°C.

If perovskite solar cells (PSCs) with high power conversion efficiencies (PCEs) are to be commercialized, they must achieve long-term stability, which is usually assessed with accelerated degradation tests. One of the persistent obstacles for PSCs has been successfully passing the damp-heat test (85°C and 85% relative humidity), which is the standard for verifying the stability of commercial photovoltaic (PV) modules. We fabricated damp heat–stable PSCs by tailoring the dimensional fragments of two-dimensional perovskite layers formed at room temperature with oleylammonium iodide molecules; these layers passivate the perovskite surface at the electron-selective contact. The resulting inverted PSCs deliver a 24.3% PCE and retain >95% of their initial value after >1000 hours at damp-heat test conditions, thereby meeting one of the critical industrial stability standards for PV modules.

Metal‐halide perovskites are rapidly emerging as an important class of photovoltaic absorbers that may enable high‐performance solar cells at affordable cost. Thanks to the appealing optoelectronic properties of these materials, tremendous progress has been reported in the last few years in terms of power conversion efficiencies (PCE) of perovskite solar cells (PSCs), now with record values in excess of 24%. Nevertheless, the crystalline lattice of perovskites often includes defects, such as interstitials, vacancies, and impurities; at the grain boundaries and surfaces, dangling bonds can also be present, which all contribute to nonradiative recombination of photo‐carriers. On device level, such recombination undesirably inflates the open‐circuit voltage deficit, acting thus as a significant roadblock toward the theoretical efficiency limit of 30%. Herein, the focus is on the origin of the various voltage‐limiting mechanisms in PSCs, and possible mitigation strategies are discussed. Contact passivation schemes and the effect of such methods on the reduction of hysteresis are described. Furthermore, several strategies that demonstrate how passivating contacts can increase the stability of PSCs are elucidated. Finally, the remaining key challenges in contact design are prioritized and an outlook on how passivating contacts will contribute to further the progress toward market readiness of high‐efficiency PSCs is presented.

The performance of state-of-the-art perovskite solar cells is currently limited by defectinduced recombination at interfaces between the perovskite and the electron and hole transport layers. These defects, most likely under-coordinated Pb and halide ions, must either be removed or passivated if cell efficiencies are to approach their theoretical limit. In this work, we introduce a universal double-side polymer passivation approach using ultrathin poly(methyl methacrylate) (PMMA) films. We demonstrate very high-efficiency (~20.8%) perovskite cells with some of the highest open circuit voltages (1.22 V) reported for the same 1.6 eV bandgap. Photoluminescence imaging and transient spectroscopic measurements confirm a significant reduction in non-radiative recombination in the passivated cells, consistent with the voltage increase. Analysis of the molecular interactions between Received: ((will be filled in by the editorial staff)) Revised: ((will be filled in by the editorial staff))

To gain insight into the properties of photovoltaic and light-emitting materials, detailed information about their optical absorption spectra is essential. Here, we elucidate the temperature dependence of such spectra for methylammonium lead iodide (CH 3 NH 3 PbI 3 ), with specific attention to its sub-band gap absorption edge (often termed Urbach energy). On the basis of these data, we first find clear further evidence for the universality of the correlation between the Urbach energy and open-circuit voltage losses of solar cells. Second, we find that for CH 3 NH 3 PbI 3 the static, temperature-independent, contribution of the Urbach energy is 3.8 ± 0.7 meV, which is smaller than that of crystalline silicon (Si), gallium arsenide (GaAs), indium phosphide (InP), or gallium nitride (GaN), underlining the remarkable optoelectronic properties of perovskites.

Perovskite/silicon tandem solar cells promise power conversion efficiencies (PCE) beyond the Shockley-Queisser limit of single-junction devices, however, their actual outdoor performance is yet to be investigated. Here we fabricate 25%-efficient two-terminal (2T) monolithic perovskite/silicon tandem solar cells and test them outdoors in a hot and sunny climate. We find that the temperature dependence of the bandgaps (Eg) of both silicon and perovskitewhich follow opposing trendsshifts the devices away from current matching for 2T tandems optimized at standard test conditions (STC, i.e., AM1.5G spectrum, 1000 W/m 2 , 25 °C). Consequently, we argue that the optimal perovskite bandgap at STC is Eg <1.68 eV (at STC

Tandem solar cells involving metal-halide perovskite subcells offer routes to power conversion efficiencies (PCEs) that exceed the single-junction limit; however, reported PCE values for tandems have so far lain below their potential due to inefficient photon harvesting. Here we increase the optical path length in perovskite films by preserving smooth morphology while increasing thickness using a method we term boosted solvent extraction. Carrier collection in these filmsas madeis limited by an insufficient electron diffusion length; however, we further find that adding a Lewis base reduces the trap density and enhances the electron-diffusion length to 2.3 µm, enabling a 19% PCE for 1.63 eV semi-transparent perovskite cells having an average near-infrared transmittance of 85%. The perovskite top cell combined with solution-processed colloidal quantum dot:organic hybrid bottom cell leads to a PCE of 24%; while coupling the perovskite cell with a silicon bottom cell yields a PCE of 28.2%.

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