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Nature Communications volume 16, Article number: 9435 (2025)
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Perovskite/silicon tandem solar cells can exceed Shockley-Queisser limit, but achieving complete coverage of 2-4 μm pyramids on industrial fully-textured silicon with solution-processed perovskite film remains challenging. We address this issue by spray-coating alumina particles onto fully-textured silicon, creating a super-hydrophilic rough surface that both enhances wet film coverage and provides guided nucleation sites. Although super-hydrophilic effect enhances wetting, it alone is insufficient to achieve complete coverage of pyramids by perovskite film. Beyond enhanced wetting, alumina particles promote uniform nucleation at particle-decorated sites across pyramids by lowering nucleation barrier and suppressing valley-preferred nucleation, which enables near-conformal deposition of perovskite film on pyramids. Additionally, alumina particles reduce nonradiative recombination and extend carrier lifetimes. Using this approach, we achieve a efficiency of 32.74% for perovskite/silicon tandem solar cells with one-step solution-processed perovskite on fully-textured silicon. This strategy offers a pathway for seamless integration of perovskite and silicon photovoltaics into high-performance tandem devices.
Perovskite/silicon tandem solar cells have attracted significant attention for their potential to deliver superior power conversion efficiencies (PCE) compared to single-junction silicon solar cells1,2,3,4,5,6. However, a key challenge lies in addressing the structural incompatibility between the thickness of perovskite films and the surface roughness of industrial fully-textured silicon solar cells7,8. While perovskite films typically have thicknesses ranging from 0.5 to 1 μm, the surfaces of industrial silicon solar cells are textured by pyramidal structures with heights of 2–4 μm7,8. This discrepancy complicates the cost-effective fabrication of efficient perovskite/silicon tandem solar cells using solution-processed perovskite films.
Several strategies have been explored to overcome these obstacles and enable the fabrication of efficient perovskite/silicon tandem solar cells9,10,11,12,13,14,15,16,17,18,19,20,21,22,23,24,25,26,27,28,29,30,31,32,33,34,35,36,37. One approach involves utilizing polished silicon wafers to mitigate surface roughness and dimensional mismatches9,10,11,12,13,14,15,16,17,18,19; however, the polishing process significantly increases the production cost and reflection loss of tandem solar cells. Another method combines vacuum deposition with solution processing to achieve conformal coating of perovskite layers on micrometer-scale fully-textured silicon substrates. Although effective, vacuum deposition is capital expenditure (CAPEX) intensive and relatively slow, has low material utilization, thereby driving up production costs20,21,22,23,24,25,26,27. A third strategy employs mildly-textured silicon with submicrometer-sized pyramids to ensure the thickness of the perovskite layer sufficiently exceeds the surface roughness of the silicon substrate28,29,30,31,32,33,34,35,36. While this technique improves coverage, it places strict constraints on the maximum allowable height of the pyramids, which can reduce production yield. A fourth approach involves engineering the surface of silicon bottom cells with hierarchical micro/nanotextures, facilitating the near-conformal deposition of perovskite films on micrometer-scale pyramids37. However, this approach requires additional etching and modifications to the industrial silicon bottom cells, potentially increasing costs and introducing recombination centers.
In this study, we present an innovative strategy to address the longstanding challenge of achieving complete perovskite coverage on industrial fully-textured silicon substrates with micrometer-scale pyramids. By spray-coating alumina (Al2O3) particles, we engineer a super-hydrophilic surface that significantly improves wet film coverage and nucleation uniformity. While previous studies have utilized particles to improve wettability38, enhance light scattering39,40, reduce nonradiative recombination41, or enable lead adsorption42, our approach uniquely employs Al2O3 particles to tackle simultaneously both wetting and nucleation challenges. We elucidate the underlying mechanism by which Al2O3 decoration modulates surface wettability and nucleation behavior: the super-hydrophilic surface promotes wet film coverage over the pyramid tips during wetting and drying, while the particles introduce small local morphology angle to reduce nucleation barrier at decorated sites, suppressing valley-dominant growth and enabling uniform nucleation across pyramid tips and sidewalls. This strategy allows the fabrication of efficient perovskite/silicon tandem solar cells on fully-textured silicon via a simple one-step solution processed perovskite deposition process.
To determine whether a super-hydrophilic surface could achieve complete coverage of solution-processed perovskite films over 2–4 μm silicon pyramids, we investigated the effects of wetting properties and nucleation dynamics. Fully-textured substrates were prepared with three surface configurations: (i) Si/2PACz, (ii) Si/NiOx, (iii) Si/NiOx/2PACz/Al2O3-particles, as illustrated in Fig. 1. Deposition details for Al2O3-particles are described in the next section. The measured contact angles of the perovskite precursor on these fully-textured surfaces were 29.0°, 4.9°, and 2.5°, respectively (Fig. 1a–c), with the latter two exhibiting super-hydrophilic behavior (contact angles < 10°). We note that minor variations in contact angle measurements are inevitable due to droplet spreading dynamics and measurement resolution, particularly for super-hydrophilic surfaces with contact angles below 10° (Supplementary Fig. 1). Nonetheless, the qualitative wetting characteristics between hydrophilic and super-hydrophilic behavior remain clearly distinguishable.
Measured contact angles of perovskite precursor on different textured substrates: a Si/2PACz, b Si/NiOx, and c Si/NiOx/2PACz/Al2O3. Cross-sectional SEM images (with tilt angle of 10°) and top-view surface SEM images of perovskite thin film deposited on different textured substrates: d, g Si/2PACz, e, h Si/NiOx, and f, i Si/NiOx/2PACz/Al2O3. j–l Schematic illustrations showing the wetting and drying as well as the nucleation and growth processes of solution-processed perovskite films on different textured substrates: j Si/2PACz, k Si/NiOx, and l Si/NiOx/2PACz/Al2O3.
For the fully-textured silicon with pyramid heights of 2–4 μm (Supplementary Fig. 2), after depositing a perovskite thin film using a 1.7 M perovskite, the tips of most large pyramids protruded through the perovskite film on the 2PACz-coated textured substrate (Fig. 1d, g). On the NiOx-coated silicon, the super-hydrophilic surface facilitated perovskite solution climbing along the pyramid sidewalls; however, complete coverage of the textured surface by perovskite film was not achieved even though super-hydrophilic surface enhances wetting behavior (Fig. 1e, h). In contrast, the incorporation of Al2O3-particles enabled near-conformal coating of 2–4 μm pyramids using a perovskite thin film of approximately 1 μm thickness (Fig. 1f, i). For textured silicon wafer with smaller pyramids (e.g., 1–2.5 μm in height), this particle-decoration strategy remains effective, enabling complete coverage of the pyramid structures by the solution-processed perovskite film, as shown in Supplementary Fig. 3.
During the wetting and drying process before nucleation occurs, super-hydrophilic surfaces outperform hydrophilic ones in maintaining a higher wet film coverage, as illustrated in Fig. 1j–l. However, during the nucleation and growth stages, preferential nucleation at pyramid valleys induces solute diffusion from the pyramid tips to the valleys, leaving the tips exposed (Fig. 1k). To address this challenge, it is crucial to ensure both enhanced wet film coverage and uniform nucleation across the entire pyramid structure—a dual requirement that is effectively fulfilled by the introduction of Al2O3 particles, as will be discussed in third section.
We conducted a detailed comparison of perovskite film coverage across various substrate configurations. Specifically, we further examined Si/NiOx/2PACz, Si/NiOx/Me-4PACz and Si/Me-4PACz without Al2O3 particles (Supplementary Fig. 4), as well as Si/NiOx/Al2O3, Si/2PACz/Al2O3, Si/Me-4PACz/Al2O3, Si/NiOx/Me-4PACz/Al2O3 and Si/NiOx/Al2O3/Me-4PACz with Al2O3 particles (Supplementary Figs. 5 and 6). Across all cases, the introduction of Al2O3 particles consistently enabled near-conformal growth of the perovskite film over 2-4 μm silicon pyramids, irrespective of the specific hole transport layer (HTL) employed (such as NiOx, 2PACz, Me-4PACz, or NiOx/SAMs bilayer). Furthermore, the fully textured bottom cell configuration with Al2O3-particle decoration, such as Si-bottom-cell/ITO/NiOx/2PACz/Al2O3, the perovskite precursor solution exhibited a contact angle below 10°, and the perovskite film was also near-conformally deposited on the textured silicon bottom cell (Supplementary Fig. 7).
We investigated methods for depositing Al2O3 particles onto textured silicon. Blade-coating a 300 nm Al2O3 suspension led to particle accumulation at the pyramid valleys, with limited deposition on the tips (Fig. 2a), due to surface tension driving the particles toward the valleys during drying process. Spin-coating proved effective for random deposition of small particles (such as 10 nm NiOx and 30 nm Al2O3) on pyramids (Supplementary Figs. 8 and 9a), but failed for larger particles (such as 100 nm and 300 nm as shown in Supplementary Figs. 9b, c), which similarly settled in the valleys. To overcome this, we developed a spray-coating method performed on heated substrates. At room temperature, spray-coated 300 nm Al2O3 particles still concentrated in the valleys (Fig. 2b). However, when the substrate was heated to 120 °C, rapid solvent evaporation prevented particle migration, enabling random distribution across pyramid tips, sidewalls, and valleys (Fig. 2c). A low-concentration of 1 wt% Al2O3 particle suspension was employed to promote sparse and isolated particle distribution, which mitigated agglomeration. Multiple spray cycles were used to average out local variations and improve overall coating uniformity. The substrate temperature and solvent system were optimized to minimize coffee-ring effect and avoid particle clustering in the valleys. This hot-substrate spray-coating approach proved effective for Al2O3 particles with average diameters ranging from 30 nm to 500 nm, consistently yielding a random and uniform coverage of Al2O3 particles that facilitated near-conformal perovskite film formation on the fully-textured silicon substrates (Supplementary Fig. 10). These results demonstrate that hot-substrate spray-coating is a general and effective method for uniformly depositing particles of various sizes on fully textured surfaces.
a SEM image of a textured substrate blade-coated with 300 nm Al2O3 particle suspension. SEM images of textured substrates spray-coated with 300 nm Al2O3 suspension at b room temperature (RT) and c 120 °C. d AFM image of a textured substrate decorated with Al2O3 particles via spray coating at 120 °C. e Comparison of calculated (lines) and measured (dots) contact angles of the perovskite precursor on flat silicon, textured silicon, and textured silicon decorated with Al2O3 particles, using different HTLs. f, g Cross-sectional SEM images of perovskite films coated with 0.25 M precursor on f Si/NiOx and g Si/NiOx/2PACz/Al2O3. h Relationship between f(β,θ) and β for nuclei with θ = 90°, with schematic illustrations of β at pyramid tips, sidewalls, valleys, and particle-decorated interfaces. i Dependence of nucleation energy (Delta {G}_{{{mathrm{het}}}}) and nucleation barrier (Delta {G}_{{{{rm{h}}}}{{{rm{e}}}}{{{rm{t}}}}}^{*}) on nucleus radius at different β values.
We further investigated the influence of particle coverage percentage on achieving complete coverage of textured silicon by perovskite film. By varying the spray volume of 1 wt% 300 nm Al2O3 suspension, we tuned surface coverage on textured silicon from ~18% to ~73% (Supplementary Fig. 11). Near-conformal perovskite film coating on fully textured substrate was obtained when the coverage ranged from ~42% to ~73%, whereas low coverage of ~18% led to incomplete coating with some pyramid tips exposed. Given this broad processing window of particle size and coverage, we selected an intermediate condition, 300 nm particles with a surface coverage of ~58% (Fig. 2c), which ensures sufficient fabrication tolerance.
In addition, the spatial distribution of Al2O3 particles can be modulated by adjusting the spray-coating incident angle. A smaller incident angle (e.g., 5°) favors particle accumulation near the pyramid tips (Supplementary Fig. 12), while larger angles (e.g., 20°) result in more randomized distribution across the entire textured surface (Fig. 2c). Notably, both tip-enriched and random distributions of particles successfully enabled near-conformal perovskite film formation (Fig. 1f and Supplementary Fig. 12), indicating that precise particle deposition in the valleys is not a prerequisite.
Incorporation of Al2O3 particles increases the surface roughness, which improves wettability on inherently hydrophilic surfaces. According to the Wenzel model, the measured contact angle on a rough surface (({theta }_{{{{rm{C}}}}}^{{prime} })) relates to that on a smooth surface (θC) by ref. 43:
where r is the roughness ratio (the ratio of actual to projected surface area). For textured silicon, the roughness ratio was 1.41 (Supplementary Fig. 13), which increased to 1.78 after spray-coating 300 nm Al2O3-particles across the pyramids, as measured by atomic force microscopy (Fig. 2d). This increased roughness ratio leads to a reduction in contact angles for the perovskite precursor across various hole transport layers (e.g., NiOx, 2PACz, Me-4PACz, or NiOx/SAMs bilayer), with calculated angles all below 10° after Al2O3-particle decoration (Fig. 2e), consistent with experimental observations (Fig. 1a–c, Supplementary Figs. 4–6).
While enhanced wettability promotes wet film coverage at the pyramid tips, the final perovskite coverage is ultimately governed by the interplay between wet film thinning and nucleation kinetics. Surface tension induces Laplace pressure on rough surface44, which causes the precursor film to naturally form a thicker layer in the valleys and a thinner one at the tips (Supplementary Fig. 14). During solvent evaporation, wetting adhesion and geometrical pinning of wet film at the pyramid tips help mitigate this thickness non-uniformity (Supplementary Fig. 14). The rough surface increases the effective liquid–solid contact area and lowers the measured contact angle, thereby enhancing wetting adhesion45. Moreover, local roughness imposes additional energy barriers for the receding contact line, thereby strengthening the pinning effect to prevent dewetting during drying46. However, if nucleation preferentially initiates in the valleys, solute migration from the tips to the valleys during drying may lead to material depletion at the pyramid tips, resulting in incomplete coverage and tip exposure.
To visualize the nucleation behavior, we reduced the precursor concentration from 1.7 M to 0.25 M to obtain discontinuous films that reveal preferred nucleation sites. On NiOx-coated substrates, nucleation predominantly occurred in the pyramid valleys, resulting in valley-concentrated grains (Fig. 2f). In contrast, upon introducing Al2O3-particle decoration, the resulting perovskite material was primarily located at particle/substrate and particle/particle interfaces, indicating suppressed valley-preferred nucleation. Interestingly, most Al2O3 particle tops remained uncovered, even though the wet film was expected to coat both the surroundings and the tops of the particles prior to nucleation. These observations highlight that nucleation dynamics—beyond wetting alone—play a critical role in determining the final film coverage. The presence of Al2O3 particles appears to lower the local nucleation barrier and promote nucleation at particle/substrate and particle/particle interfaces. This particle-guided nucleation behavior was consistently observed across various HTL configurations, including Si/NiOx/Al2O3, Si/Me-4PACz/Al2O3, Si/NiOx/Me-4PACz/Al2O3, and Si/NiOx/Al2O3/Me-4PACz, as shown in Supplementary Fig. 15.
When nucleation and growth at particle-decorated sites occur before the wet film levels out—particularly at a high precursor concentration of 1.7 M—the film remains slightly thicker in the valleys and achieves near-conformal and complete coverage. At a lower precursor concentration of 0.5 M, the extended drying time allows the wet film to homogenize in thickness before nucleation, resulting in a perovskite layer approximately 200 nm thick with conformal coverage across most of the particle-decorated textured surface (Supplementary Fig. 16).
The variation in nucleation barriers across different locations on a rough surface arises from the morphology factor f(β,θ). The energy of heterogeneous nucleation ((Delta {G}_{{{{rm{het}}}}})) and critical heterogeneous nucleation energy ((Delta {G}_{h{{{rm{e}}}}t}^{*})) depends on f(β,θ)47:
where (Delta {G}_{hom }^{*}) is critical homogeneous nucleation energy, β is the local morphology angle, θ is the nucleus contact angle on the substrate, ({gamma }_{{{{rm{SL}}}}}) is the nucleus–liquid interfacial energy, Ω is the monomer volume, k is Boltzmann’s constant, T is temperature, and σ is the degree of supersaturation. For typical textured silicon pyramids, β reduces from ~290° at tips to ~180° on sidewalls and further to ~70° at valleys. As shown in Fig. 2h, f(β,θ) is significantly lower at the valleys, favoring valley-preferred nucleation, and solute migration to these regions during drying could leave the tip areas exposed even if initially wetted (illustrated in Fig. 1k).
Particle decoration could introduce small local morphology angle β to modulate the nucleation behavior. Although the contact angle θ varies slightly with different HTL configurations, its effect on nucleation behavior is negligible in Al2O3-decorated samples, as observed in Supplementary Fig. 15. The dominant factor enabling particle-guided nucleation is β. The introduction of Al2O3 particles could significantly reduce β at particle–substrate and interparticle interfaces to below 30°, resulting in a corresponding drop in f(β,θ) value to less than 0.017—substantially lower than the values at pyramid tips (~0.91), sidewalls (~0.5), or valleys (~0.09) for θ = 90°, as illustrated in Fig. 2h. This reduction in f(β,θ) dramatically lowers the nucleation barrier (Delta {G}_{{{{rm{h}}}}{{{rm{e}}}}{{{rm{t}}}}}^{*}) at particle–substrate and interparticle interfaces (as illustrated in Fig. 2i)47,48,49, thereby promoting nucleation at particle-decorated interfaces.
In summary, Al2O3-particle decoration fulfills two critical roles: it enhances wet film coverage at the pyramid tips via increased wettability, and it facilitates uniform nucleation across the textured surface by reducing the nucleation barrier and suppressing valley-preferred nucleation. This dual mechanism enables near-conformal perovskite film coverage on fully textured silicon substrates.
The particle decoration strategy remains effective across different perovskite precursor systems. Besides typical mixed solvents of DMF:DMSO (4:1 v/v), we also evaluated other solvents—DMF:NMP (4:1 v/v), and 2-ME:DMF:DMSO (3:1:1 v/v/v). As shown in Fig. 2e and Supplementary Fig. 17, their contact angle on flat Si/NiOx/2PACz substrates is 49.6°, 47.1°, and 42.2°, respectively, reflecting differences in surface tension and solvent–substrate interactions. Despite these variations, all formulations achieved near-conformal perovskite films on textured silicon with Al2O3 particles (Supplementary Fig. 17). Furthermore, X-ray photoelectron spectroscopy (XPS) confirms that Al2O3 particles do not chemically react with either the SAM layers or the perovskite precursor (Supplementary Fig. 18). This indicates that the primary function of particle-guided growth is attributed to the morphological effect rather than solvent properties or chemical bonding.
We investigated the impact of Al2O3-particle decoration on carrier transport behavior in perovskite films. Perovskite films deposited on Al2O3-particle spray-coated glass substrates exhibited stronger steady-state photoluminescence (PL) intensity compared to control films deposited on bare glass (Fig. 3a). Time-resolved PL (TRPL) measurements further revealed a longer radiative recombination lifetime for the particle-decorated film (1.90 μs vs. 1.47 μs for control, Fig. 3b). Quasi-Fermi level splitting (QFLS) values, derived from photoluminescence quantum yield (PLQY) measurements, under varying illumination intensities (Suns-QFLS) showed higher QFLS in the particle-decorated films than in the control films (Fig. 3c). Moreover, the diode ideality factor, calculated from the Suns-QFLS plots, decreased from 1.40 in the control films to 1.36 in the particle-decorated films. In addition, trap density of states (t-DOS) analysis confirmed the reduction of defect density after incorporation of Al2O3 particles (Supplementary Fig. 19). To differentiate bulk and surface recombination effects, TRPL measurements as a function of film thickness were analyzed using the reported double heterostructure model38,41,50. This analysis revealed an increase in bulk lifetime (τb) from 2.99 to 3.68 µs and a reduction in surface recombination velocity (SRV) from 22.03 to 12.67 cm/s for films deposited on particle-decorated substrates (Fig. 3d). SEM images in Supplementary Fig. 20 show that the presence of Al2O3 particles at interface does not substantially influence the grain size of perovskite film. These results show that Al2O3-particles suppress both bulk and surface recombination, consistent with previous reports on the reduction of nonradiative recombination in perovskite solar cells using porous insulating contacts41. This improvement is likely attribute to the hydrophilic and rough surface properties of Al2O3 particles, which influence the growth dynamics and bulk quality of the perovskite film41.
a Steady-state PL spectra, b TRPL spectra, c Suns-QFLS plots for glass/perovskite and glass/Al2O3/perovskite samples. d Bulk lifetime (τb) and SRV of the glass/perovskite and glass/Al2O3/perovskite samples by fitting the TRPL decays of perovskite film with varied thicknesses. e J–V curves and f PCE statistics of single junction perovskite solar cells fabricated on glass/ITO/NiOx/2PACz without and with Al2O3-particle decoration. Box range is standard deviation and center line is median.
We evaluated the influence of Al2O3-particle decoration on the performance of single-junction perovskite solar cells with the device architecture of glass/ITO/NiOx/2PACz/with or without Al2O3/perovskite/C60/BCP/Cu. For these single-junction devices with Al2O3-particles, the particle surface coverage was adjusted to close to 58% (Supplementary Fig. 21), which is comparable to the coverage used on the textured silicon substrates in the tandem devices. Compared to the control devices without Al2O3-particles, those incorporated with Al2O3-particles demonstrated a slight enhancement in open-circuit voltage (VOC), increasing from 1.249 V to 1.261 V, along with a modest improvement in PCE, rising from 21.14% to 21.80% (Fig. 3e). These improvements were further validated through statistical analysis of device performance (Fig. 3f and Supplementary Fig. 22).
We fabricated perovskite/silicon tandem solar cells using heterojunction silicon bottom cells with fully-textured pyramids on both surfaces. The device structure is illustrated in Fig. 4a, where Al2O3-particles were spray-coated onto the NiOx/2PACz HTL-coated silicon bottom cells with ITO intermediate layer, and the solution-processed perovskite films were dried by gas-pump method. For cross-sectional SEM characterization of mechanically cleaved samples, void-like features were occasionally observed at the perovskite/substrate interface due to the displacement of Al2O3 particles during mechanical cleaving (Supplementary Fig. 23). To obtain more representative structural information, we employed focused ion beam (FIB) milling to prepare cross section. The FIB-prepared cross-sectional image confirms the presence of Al2O3 particles at interface and reveals a near-conformal and compact perovskite layer on the textured silicon cell (Fig. 4b). With Al2O3-particle decoration, the champion tandem solar cell achieved a PCE of 32.77%, with a VOC of 1.966 V, a short-circuit current density (JSC) of 20.39 mA/cm2, and a fill factor (FF) of 81.76% (Fig. 4c and Supplementary Table 1), and the steady-state power output was 32.74% (Supplementary Fig. 24). The dark J–V characteristics exhibited ideal diode behavior (Supplementary Fig. 25). One of the tandem devices assessed by a third party exhibited a PCE of 32.69% under dual-light solar simulator calibrated with provided EQE and certified reference silicon cell (Supplementary Fig. 26). In contrast, tandem devices fabricated without Al2O3 decoration exhibited low PCEs of around 15% (Fig. 4c, d), due to incomplete perovskite coverage on the fully-textured pyramids. The tandem solar cells with Al2O3-particles exhibited no hysteresis in the J–V scans (Fig. 4e). The measured JSC showed good agreement with the integrated current density calculated from the EQE data (Fig. 4f).
a Schematic illustration of perovskite/silicon tandem solar cell on fully-textured silicon with Al2O3-particle decoration. b FIB-prepared cross-sectional SEM image (with tilt angle of 35°) of perovskite/silicon tandem solar cell. A thick protective layer of ~ 1.1 μm IZO was deposited on top of tandem device to mitigate “waterfall” effect commonly observed in FIB milling. c J–V curves and d PCE statistics of perovskite/silicon tandem solar cells fabricated on fully-textured substrate without and with Al2O3-particle decoration. Box range is standard deviation and center line is median. e J–V curves and photovoltaic parameters of the tandem solar cell under reverse and forward scans. f EQE and total absorptance (1−R, where R is the reflectance) of the tandem cell.
Notably, besides NiOx/2PACz/Al2O3, high-efficiency perovskite/silicon tandem devices were achieved across various HTL configurations upon inclusion of Al2O3 particles, such as NiOx/Me-4PACz/Al2O3 and Me-4PACz/Al2O3 (Supplementary Fig. 27 and Supplementary Table 2). Although NiOx is not essential for near-conformal perovskite coverage in the presence of Al2O3, its incorporation improves surface wettability and enhances HTL uniformity51, leading to slightly better device performance.
To assess the influence of Al2O3 coverage percentage on device performance, we varied the spray volume to achieve coverage levels ranging from ~42% to ~73%. Within this range, the perovskite films consistently exhibited near-conformal coating over the fully textured pyramids, as discussed in the previous section (Supplementary Fig. 11). The corresponding tandem devices all achieved PCEs exceeding 32% (Supplementary Fig. 28 and Supplementary Table 3). This large window of Al2O3-particle coverage for high-efficient tandem solar cells enables a narrow PCE distribution for the fabricated tandem solar cells.
The sprayed Al2O3 particles demonstrated small absorption across the relevant wavelength range (Supplementary Fig. 29). EQE measurements indicated that increasing Al2O3 coverage had no significant impact on the photocurrent generated by the silicon bottom cell (Supplementary Fig. 28), which is likely due to a balance between enhanced light scattering and parasitic absorption introduced by the Al2O3 particles.
In addition to the gas-pump method, we further demonstrated that complete perovskite film deposition on fully textured substrates can also be achieved using anti-solvent method. As shown in Supplementary Fig. 30, this approach enabled the deposition of ~1 μm-thick near-conformal perovskite layers and yielded tandem devices with PCEs over 32%. Under anti-solvent processing with a 0.25 M precursor concentration, Al2O3-particle decoration facilitated preferential nucleation at particle-decorated sites, whereas in the absence of Al2O3, nucleation predominantly occurred in the pyramid valleys (Supplementary Fig. 31). As illustrated in Fig. 2h, the morphology factor f(β,θ) at particle/substrate and interparticle interfaces can be over 20 times lower than that of conventional flat surfaces. This pronounced difference allows particle-decorated interfaces to influence nucleation behavior during anti-solvent drying, thereby facilitating near-conformal perovskite film growth on textured substrates.
The incorporation of Al2O3 particles does not appear to compromise device stability, instead, it slightly enhances stability, as shown in single-junction devices in Supplementary Fig. 32, consistent with the effect of prior reported porous Al2O3 insulating contact41. However, the operational stability of perovskite solar cells and tandem devices in this study remains insufficient. After 500 h of continuous operation under 100 mW/cm2 illumination of LED-based solar simulator at room temperature in a nitrogen atmosphere, the unencapsulated tandem device incorporating Al2O3 particles retained 90.1% of its initial PCE (Supplementary Fig. 33). The relatively fast degradation of the perovskite cells and tandem devices may be attributed to the residual PbI2 in the perovskite film (Supplementary Fig. 34), which has been reported to accelerate degradation under operational conditions52,53,54. While long-term operational stability falls outside the main scope of this work, it will be a key focus of our future research efforts.
This particle-decoration strategy supports diverse HTL architectures, broad particle coverage ranges, and various perovskite deposition methods. Importantly, it does not require changes to the industrial fully-textured silicon solar cell process, offering a simple and scalable one-step solution-based route for integrating perovskite and silicon photovoltaics into tandem solar cell technologies.
In this study, we addressed the challenge of achieving complete coverage of micrometer-scale pyramids on fully-textured silicon solar cells with one-step solution-processed perovskite films. By spray-coating alumina particles, we created a super-hydrophilic interface that not only enhanced wetting behavior but also redirected nucleation dynamics, enabling near-conformal perovskite film growth across the fully-textured silicon surface. The improved wetting ensured completely coverage of wet film on the pyramids prior to dry film formation. Additionally, alumina particles effectively suppressed valley-preferred nucleation by promoting nucleation at particle-decorated sites on pyramid tips and sidewalls, overcoming the inherent energy disparities that favor nucleation at pyramid valleys. Without this redirection of nucleation dynamics, super-hydrophilicity alone would fail to achieve complete coverage after the nucleation and growth process. Moreover, the incorporation of alumina particles mitigated nonradiative recombination and enhanced carrier lifetimes. These advancements enabled the fabrication of perovskite/silicon tandem solar cells with a power conversion efficiency of 32.74%, using a simple one-step solution-processed method. This strategy offers a cost-effective pathway for the integration of perovskite and silicon photovoltaics, accelerating the development of high-performance tandem solar technologies and expanding their commercial adoption.
Formamidinium iodide (FAI), methylammonium chloride (MABr), cesium iodide (CsI), and propane-1,3-diammonium iodide (PDAI2) were purchased from Greatcell Solar. Al2O3 particles were purchase from Dashinou Nanotechnology (Changzhou) Co., Ltd. Lead iodide (PbI2), (2-(9H-carbazol-9-yl)ethyl)phosphonic acid (2PACz), (4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl)phosphonic acid (Me-4PACz) were purchased from TCI. Lead bromide (PbBr2), lithium fluoride (LiF), N,N-dimethylformamide (DMF), dimethyl sulfoxide (DMSO), N-Methyl-2-pyrrolidone (NMP), 2-Methoxyethanol (2-ME), anisole, isopropanol (IPA) were purchased from Sigma Aldrich. C60 and bathocuproine (BCP) were purchased from Xi’an Yuri Solar Co., Ltd. Nickel oxide (NiOx) nanoparticles were purchased from Advanced Election Technology Co., Ltd. All the chemicals were used as received without further purification.
Fully-textured silicon substrates were cleaned by spin coating IPA at 3000 rpm for 30 s. For self-assembled monolayers (SAMs) coated silicon, after UV-O3 treatment, 2PACz or Me-4PACz (0.8 mg/mL in IPA) solution was spin-coated onto silicon at 3000 rpm for 30 s, annealed at 100 °C for 5 min in a nitrogen-filled glovebox, washed by spin coating IPA at 3000 rpm for 30 s, and then annealed at 100 °C for 5 min. For NiOx coated silicon, NiOx was deposited by spin-coating NiOx nanoparticle ink (with particle diameter of ~10 nm, 10 mg/mL in deionized water) on UV-O3 treated silicon at 4000 rpm for 30 s, followed by annealing at 150 °C for 20 min in air. For NiOx/SAMs coated silicon, following NiOx deposition, 2PACz or Me-4PACz was deposited as described above.
Al2O3-particle suspensions (1 wt% in IPA, with average diameter of 30 nm, 100 nm, 300 nm, or 500 nm) were ultrasonicated for 30 min prior to coating. As shown in Supplementary Fig. 35, spray coating was performed using a custom-built spray setup (with Iwata Eclipse HP-CS airbrush, a gravity-feed, dual-action model) operated at 0.1 MPa with an incident angle of ~20°. The airbrush was positioned ~15 cm away from the samples, and substrates were heated to 120 °C during spray-coating. The spray direction was sequentially rotated to face each of the four pyramid sidewalls. Each spray pass covered a distance of ~10 cm at a speed of approximately 10 cm/s. Different volumes of suspension were sprayed to tune the surface coverage of Al2O3 particles. For fully-textured silicon, 12 mL of 1 wt% 300 nm Al2O3 suspension was sprayed for one batch of textured samples.
For the spin-coating method, the sample was coated with a 2 wt% Al2O3 particle suspension at 2000 rpm for 30 s, followed by annealing at 120 °C for 5 min. For the blade-coating method, the sample was coated with a 2 wt% Al2O3 particle suspension at a speed of 25 mm/s with a gap of 100 μm, and subsequently annealed at 120 °C for 5 min.
A 1.7 M perovskite precursor solution of Cs0.05MA0.15FA0.80Pb1.015(I0.755Br0.255)3 was prepared by dissolving CsI, FAI, MABr, PbBr2, and PbI2 in a DMF:DMSO (4:1 v/v) mixed solvent. The solution was stirred for 8 h and filtered through a 0.22-μm PTFE filter before use. The perovskite films were deposited on textured silicon with different types of HTLs with and without Al2O3-particle decoration using the gas-pump method47, where the precursor was spin-coated at 500 rpm for 5 s and 4000 rpm for 20 s, followed by drying at 0.1 Pa for 60 s using a gas pump crystallizer (GPC0001J, Kaifu). The samples were subsequently annealed at 65 °C for 1 min and then at 100 °C for 30 min. For 0.25 M and 0.5 M perovskite precursor in mixed DMF:DMSO (4:1 v/v), the precursor was spin-coated at 500 rpm for 5 s and 2000 rpm for 10 s, followed by gas pumping and thermal annealing.
For the sample prepared by anti-solvent method, the precursor was spin-coated in three steps: 500 rpm for 5 s, 2000 rpm for 90 s, and 7000 rpm for 10 s, and 500 μL anisole was applied at 8 s before the end of spin-coating process. The samples were then annealed at 65 °C for 1 min, followed by 100 °C for 30 min.
For perovskite precursor with different mixed solvents, 1.7 M perovskite precursor was prepared using either DMF:NMP (4:1 v/v) or 2-ME:DMF:DMSO (3:1:1 v/v/v) as solvent. The perovskite films were deposited via spin coating followed by the gas-pump drying method as described above.
ITO glass substrates were cleaned by ultrasonication sequential in acetone, IPA, and ethanol for 20 min each. After 30 min of UV-O3 treatment, NiOx and 2PACz were deposited as described above. Al2O3 particles were spray-coated onto the ITO/NiOx/2PACz substrates. After deposition of perovskite film by 1.7 M precursor via spin coating, gas pumping and thermal annealing, a PDAI2 solution (0.5 mg/mL in IPA) was spin-coated onto the annealed films at 4000 rpm for 30 s, followed by annealing at 100 °C for 10 min. Finally, 25 nm of C60 was deposited at 0.1 Å/s, followed by 4 nm of BCP at the same deposition rate, and 100 nm of Cu at 1.0 Å/s using thermal evaporation.
For silicon bottom cell fabrication, silicon heterojunction bottom cells were fabricated on n-type double-side fully-textured monocrystalline silicon wafers (CZ, 210 mm×210 mm, 1–5 Ω resistivity, 150 μm thickness). The intrinsic, n-type and p-type hydrogenated amorphous silicon layers were deposited on each side of the wafer using plasma-enhanced chemical vapor deposition (PECVD). Following PECVD, ITO layers (~80 nm rear, ~20 nm front) were sputtered through a shadow mask (10.5 cm × 10.5 cm), followed by screen-printed Ag electrodes at the rear. Wafers were laser-cut to 2.5 cm × 2.5 cm substrates for tandem fabrication. The silicon bottom cells were fabricated by Zhejiang Aiko Solar Energy Technology Co., Ltd.
Fully-textured silicon bottom cells were cleaned by spin-coating IPA at 3000 rpm for 30 s. After UV-ozone treatment, NiOx deposition, 2PACz coating, Al2O3 particle spray-coating, perovskite deposition, and surface passivation as described above, a 15 nm C60 layer was deposited by thermal evaporation at 0.1 Å/s. A 10 nm SnO2 layer was deposited by atomic layer deposition (ALD) at 100 °C for 80 cycles (TALD-150D, Jiaxing Kemin Electronic Equipment Technology Co., Ltd.). The IZO top electrode, with a thickness of 70 nm, was sputtered onto the SnO2 buffer layer. Finally, top Ag fingers (150 nm thick) were thermally evaporated through a shadow mask, and 100 nm of LiF antireflection coating was deposited at a rate of 1 Å/s to complete the tandem devices.
The contact angle measurements were conducted using a KRUSS DSA 100 instrument. A field-emission scanning electron microscope (FEI VERIOS 460) was used to examine the surface and cross-sectional morphologies of the films. Most of cross-sectional samples were prepared by mechanically cleaving the silicon wafers. The cross-section prepared by FIB milling was conducted using Helios Nanolab 600i, and ~1.1 μm IZO was deposited on top of tandem device as protection layer to mitigate “waterfall” effect during FIB milling. Energy dispersive X-ray spectroscopy (EDS) was conducted using MIRA3 LMH (TESCAN). Atomic force microscopy (AFM) measurements were performed using an INNOVA atomic force microscope. Steady-state photoluminescence (PL) and time-resolved photoluminescence (TRPL) spectra were measured using a Horiba DeltaFlex spectrometer with an excitation wavelength of 405 nm. Photoluminescence quantum yield (PLQY) measurements were conducted with an LuQY Pro LP20-32 radiative efficiency meter (QYB) under varying illumination intensities. Suns-QFLS analysis was performed according to established methods55. t-DOS measurements were performed by using an Agilent E4980A precision LCR meter, with scanning range of AC frequency from 0.02 to 200 kHz and amplitude of AC bias of 20 mV. XPS measurements were conducted using Thermo Fisher ESCALAB Xi+ system. Absorption measurement was performed by PE Lambda950.
The J–V characteristics of single-junction and tandem solar cells were measured at room temperature in an ambient environment. A Keithley 2400 source meter and a calibrated Wavelabs Sinus 220 LED-based solar simulator with an AM1.5 G irradiance spectrum were used for the measurements. The Wavelabs Sinus 220 LED-based solar simulator was calibrated to 1-sun intensity (100 mW cm−2) using three reference silicon cells, each calibrated by the Fujian Metrology Institute: 1) with a KG5 filter on May 13, 2024, 2) with a KG2 filter on August 2, 2024, and 3) with a quartz filter on October 9, 2023. The aperture area of the single-junction perovskite solar cells was defined by a photomask with an aperture of 0.0544 cm2, while that for tandem solar cells was 1.0037 cm2. Each device was exposed to light for 10 s before J–V scan. For single-junction solar cells, J–V curves were recorded over a voltage range of 1.3 V to -0.1 V with a 10 mV step size and a delay of 500 ms. For tandem solar cells, J–V curves were measured over a voltage range of 2.1 V to -0.2 with a 20 mV step size and a delay of 500 ms. The stability measurements were performed at the maximum power point (MPP) under 100 mW/cm2 illumination of LED-based solar simulator (LST-LED20, Shanghai Jinzhu Technology Co., Ltd.) at room temperature in N2-filled gloveboxes using an MPP tracking algorithm (Shenzhen Purui Material Technology Co., Ltd.). External quantum efficiency (EQE) and 1 − R were acquired using Enlitech’s QE-R system. For measuring the EQE of perovskite top cells, the tandem devices were light-biased using white light equipped with an Enlitech L850 U long-pass filter (cut-off wavelength: 850 nm). For measuring the EQE of silicon bottom cells, the tandem devices were light-biased using white light equipped with an Enlitech S550 U short-pass filter (cut-off wavelength: 550 nm). The spectra irradiance for Wavelabs light source was measured using an external spectrometer (Maya2000, Ocean Optics), and the mismatch factors for both sub-cells were around 1.00 ± 0.01.
Further information on research design is available in the Nature Portfolio Reporting Summary linked to this article.
All data generated in this study are provided in the main text, Supplementary Information, and Source Data file. Source data are provided with this paper.
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This work was financially supported by the National Natural Science Foundation of China (Grant No. 52273273, B.C.) and Qin Chuang Yuan project (Grant No. QCYRCXM-2023-081, B.C.). We gratefully acknowledge the FIB support provided by senior engineer Qinqin Fu from the School of Materials Science and Engineering, Xi’an Jiaotong University.
These authors contributed equally: Naihe Liu, Gao Zhang, Meng Wei, Lijun Yang.
School of Materials Science and Engineering, Xi’an Jiaotong University, Xi’an, Shaanxi, China
Naihe Liu, Gao Zhang, Meng Wei, Lijun Yang, Lirong Zeng, Xin Zhang, Yuwei Geng, Ying Zhu, Chengxia Shen, Yongyi Wu, Tao Li, Wei Wang, Guanjun Yang & Bo Chen
Department of Applied Physical Sciences, The University of North Carolina at Chapel Hill, Chapel Hill, NC, USA
Hangyu Gu, Jinsong Huang & Bo Chen
Zhejiang Aiko Solar Energy Technology Co. Ltd., Jinhua, Zhejiang, China
Xiaolei Li, Kaifu Qiu & Peicheng Wei
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B.C. and J.H. conceived the idea. B.C. and G.Y. designed and supervised the research. M.W., L.Y., L.Z., and C.S. fabricated perovskite solar cells. N.L. and H.G. optimized particle deposition conditions. N.L., M.W., and L.Y. fabricated tandem solar cells. G.Z. conducted the nucleation mechanism analysis. X.Z. conducted the MPP tracking. X.L., K.Q., and P.W. fabricated silicon bottom cells. Y.G. performed the PLQY and QFLS characterization. W.W. and N.L. conducted the SEM and EDS measurement. L.Z. and Y.Z. conducted PL and TRPL measurement. Y.W. and T. L. conducted AFM measurement. B.C., N.L., G.Z., and J.H. wrote the paper, and all authors reviewed the paper.
Correspondence to Guanjun Yang, Jinsong Huang or Bo Chen.
The authors declare no competing interests.
Nature Communications thanks Anand Subbiah, and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. A peer review file is available.
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Liu, N., Zhang, G., Wei, M. et al. Particle decoration enables solution-processed perovskite integration with fully-textured silicon for efficient tandem solar cells. Nat Commun 16, 9435 (2025). https://doi.org/10.1038/s41467-025-64546-0
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