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.

Polymer aggregation and crystallization behavior play a crucial role in the performance of all-polymer solar cells (all-PSCs). Gaining control over polymer self-assembly via molecular design to influence bulk-heterojunction activelayer morphology, however, remains challenging. Herein, we show a simple yet effective way to modulate the selfaggregation of the commonly used naphthalene diimide (NDI)-based acceptor polymer (N2200), by systematically replacing a certain amount of alkyl side-chains with compact bulky side-chains (CBS). Specifically, we have synthesized a series of random copolymer (PNDI-CBS x ) with different molar fractions (x = 0−1) of the CBS units and have found that both solution-phase aggregation and solid-state crystallinity of these acceptor polymers are progressively suppressed with increasing x as evidenced by UV−vis absorption, photoluminescence (PL) spectroscopies, thermal analysis, and grazing incidence X-ray scattering (GIWAXS) techniques. Importantly, as compared to the highly self-aggregating N2200, photovoltaic results show that blending of more amorphous acceptor polymers with donor polymer (PBDB-T) can enable all-PSCs with significantly increased PCE (up to 8.5%). The higher short-circuit current density (J sc ) results from the smaller polymer phase-separation domain sizes as evidenced by PL quenching and resonant soft X-ray scattering (R-SoXS) analyses. Additionally, we show that the lower crystallinity of the active layer is less sensitive to the film deposition methods. Thus, the transition from spin-coating to solution coating can be easily achieved with no performance losses. On the other hand, decreasing aggregation and crystallinity of the acceptor polymer too much reduces the photovoltaic performance as the donor phase-separation domain sizes increases. The highly amorphous acceptor polymers appear to induce formation of larger donor polymer crystallites. These results highlight the importance of a balanced aggregation strength between the donor and acceptor polymers to achieve high-performance all-PSCs with optimal active layer film morphology.

Long-chain saturated hydrocarbons and alkoxysilanes are ligands that are commonly used to passivate perovskite quantum dots (PQDs) to enhance their stability and optical properties. However, the insulating nature of these capping ligands creates an electronic energy barrier and impedes interparticle electronic coupling, thereby limiting device applications. One strategy to solve this problem is the use of short conductive aromatic ligands that allow delocalization of the electronic wave function from the PQDs, which, in turn, facilitates charge transport between PQDs by lowering the energy barrier. This is demonstrated with methylammonium lead bromide (MAPbBr 3 ) QDs prepared using benzylamine (BZA) and benzoic acid (BA) capping ligands. Optimized BZA-BA-MAPbBr 3 QDs are highly stable and show very high photoluminescence (PL) quantum yield (QY) (86%). More importantly, the BZA-BA-MAPbBr 3 QD film exhibits higher conductivity and carrier lifetime and more efficient charge extraction compared to PQDs with insulating ligands, as indicated by electrochemical measurements and transient photocurrent and photovoltage spectroscopy.

In recent years, hybrid perovskite solar cells (HPSCs) have received considerable research attention due to their impressive photovoltaic performance and low-temperature solution processing capability. However, there remain challenges related to defect passivation and enhancing the charge carrier dynamics of the perovskites, to further increase the power conversion efficiency of HPSCs. In this work, the use of a novel material, phenylhydrazinium iodide (PHAI), as an additive in MAPbI 3 perovskite for defect minimization and enhancement of the charge carrier dynamics of inverted HPSCs is reported. Incorporation of the PHAI in perovskite precursor solution facilitates controlled crystallization, higher carrier lifetime, as well as less recombination. In addition, PHAI additive treated HPSCs exhibit lower density of filled trap states (10 10 cm −2 ) in perovskite grain boundaries, higher charge carrier mobility (≈11 × 10 −4 cm 2 V −1 s), and enhanced power conversion efficiency (≈18%) that corresponds to a ≈20% improvement in comparison to the pristine devices.

Tin-based halide perovskite solar cells (PSCs) hold the most promise among lead-free PSCs, but they are plagued with inadequate environmental stability and power-conversion efficiency (PCE). Here we demonstrate that the optimum incorporation of a bulky divalent organic cation, 4-(aminomethyl)­piperidinium (4AMP), in FASnI3 thin films improves stability, optoelectronic properties, and PSC performance. The optimized PSC yields a maximum PCE of 10.9% and good 500-h operational stability under continuous illumination. This is attributed to the unique thin-film structure, where the strong ionic bonding afforded by divalent 4AMP may provide near-full-coverage functionalization (encapsulation) of FASnI3 grain surfaces and grain boundaries, retarding O2/H2O ingression and mitigating Sn-defects for reduced photocarrier nonradiative recombination.