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Nature Communications volume 16, Article number: 7173 (2025)
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Wide-bandgap perovskite is pivotal as a photoactive layer in the top cell of prevailing tandem solar cells. However, the intrinsic instability of wide-bandgap perovskite solar cells is predominantly attributed to the vacancy defects caused by multiple ion migration. Here, we incorporate an ether ring super-molecule into perovskite. This supramolecular approach effectively manipulates the crystallization kinetics and suppresses the halide segregation under illumination by tuning the coordination of halides toward monovalent cations and lead ions. As a result, the supramolecular engineered 1.77 eV perovskite solar cells achieve a champion power conversion efficiency of 21.01% with an outstanding operational stability, retaining 95% of initial efficiency after 1000 h σof maximum-power-point tracking test. Meanwhile, the two-terminal all-perovskite tandem solar cells achieve the champion efficiency of 28.44% (certified 27.92%). This work paves an avenue to improve the film quality and illumination stability of mixed halide wide-bandgap perovskites with a supramolecular approach.
Single-junction perovskite solar cells (PSCs) have been certified to catch up with silicon solar cells in terms of power conversion efficiency (PCE)1. Ever-increasing efficiency is the foremost guarantee to reduce the cost of commercialized solar cells2. As the mainstream technology route for next-generation ultra-high-efficiency solar cells3, the PCE of tandem solar cells (TSCs) has exceeded the Shockley-Queisser (S-Q) limit of single-junction solar cells (33.7%)4. However, the theoretical limit efficiency of double-junction TSCs is up to 43%, which means that there is still a tremendous potential for improvement of the TSCs5. Amongst the tandem devices, the top wide bandgap (WBG) PSCs play a crucial role in synergizing with the bottom narrow-bandgap (NBG) solar cell to make full use of the sunlight and reducing thermalization losses6. In addition, WBG PSCs are attractive for building-integrated PVs (BIPVs) due to the well-responding to ultraviolet (UV) sunlight and the esthetics of the semi-transparent features7,8. However, the degradation precipitated by external stimuli, including light, heat, and humidity, remains a pivotal obstacle for WBG PSCs in pursuit of real-world applications9.
Analogous to other perovskite, the organic-inorganic hybrid WBG perovskite has a soft lattice structure on account of relatively weak ionic bonding between metal cation and halide anion, as well as the non-covalent bonding between organic ammonium cations and inorganic framework octahedrons, and the bonds between the metal/organic cations and the halogens are prone to fracture in response to external stimuli10. For the ABX3-typical mixed-halide WBG perovskite, the migration activation energy of the halogen anion (0.1 eV) at the X-site is lower than that of the cation (0.5 eV) at the A-site and the metal cation (0.8 eV) at the B-site11,12, which indicated that the halogen anion undergoes ionic migration rather susceptibly13. The WBG bromine-rich (Br-rich) and NBG iodine-rich (I-rich) regions are easily formed under illumination due to the different migration rates and electronegativity of I and Br ions14. The Br-rich region has a high defect density and many deep-level defects, and the I-rich region is susceptible to hole trapping and oxidation, becoming a charge recombination center and trapping photogenerated carriers15. As a result, the inhomogeneous segregation of ions causes massive bulk and interfacial defects12, inducing strong nonradiative recombination16, leading to a decrease in steady-state output power and quasi-Fermi energy level splitting, which ultimately leading to an open-circuit voltage loss17, thus degrading the photovoltaic performance and stability of the WBG PSCs along with limiting the efficiency and lifetime of the TSCs18,19,20.
Aiming to fabricate highly efficient and stable TSCs, the WBG perovskite were optimized by refining the composition of ingredients21, preparation methods (e.g., spinning22, blade-coating23, gas quenching24, spraying, flashing25, physical vapor deposition26, etc.), and additives engineering (e.g., organic salts27 natural molecules28, small molecules29 and supramolecular agents30, etc.). Notably, supramolecular crown ethers outperform low-dimensional long-chain organic salts by offering distinctive benefits in precursor stabilization, lattice-matched coordination, and host-guest complexation31,32. Macrocyclic crown ethers can adjust their coordination ability with different metal ions by the type and number of donor atoms or the size of the ring33. Meanwhile, crown ethers can also form halogen bonds directly with halogen anions34. These attributes may play a pivotal role in substantially improving the efficiency and reproducibility of PSCs.
Herein, we utilized macrocyclic dibenzo-30-crown-10 (DB30C10) molecules as an additive to modify the WBG perovskite by tuning the coordination of halides toward monovalent cations and lead ions. The oxygen-enriched large ether ring of DB30C10 interacted with formamidine (FA+) and cesium (Cs+) cations at the A-site, along with undercoordinated Pb2+ at the B-site, synergistically regulated the ionic migration of the halogens at the X-site. Consequently, DB30C10-modified perovskite significantly reduced defect density, suppressed mixed-halogen segregation and inhibited nonradiative recombination of photo-generated carriers both in the bulk and at the interfaces, which enhanced PCE and stability in WBG PSCs and TSCs. The champion efficiencies of opaque and semi-transparent 1.77 eV-bandgap DB30C10-modified PSCs achieved 21.01% and 18.97%, respectively, while the four-terminal (4 T) and two-terminal (2 T) all perovskite tandem cells yielded remarkable efficiencies of 28.37% and 28.44%, respectively.
Enhancing the Br content of perovskite precursor is a direct and widely adopted technique for obtaining WBG perovskites7. Compared to conventional bandgap perovskites, Br-rich WBG perovskites prepared via solution methods exhibit faster crystallization rates, attributed to the smaller ionic radius and lower nucleation energy of Br ions relative to I ions35. In mixed-halide WBG perovskite, the initially homogeneous halogen-distributed state has the lowest formation energy in the dark36. Upon stimulation by light, heat, and humidity, the I and Br ions with relatively low mobility energies were subjected to ionic migration through uncoordinated vacancy defects (e.g., VFA, VCs, and VPb), ultimately giving rise to phase separation of I-rich and Br-rich regions37. Regulation by coordination chemistry is essential for perfecting the crystallization of WBG perovskites crystals, controlling the emergence of vacancy defects, and achieving homogeneity of perovskite films38. Crown ethers, unlike popular long-chain organic ligands, are macrocyclic ether organic ligands whose cavity size increases with the number of electron-rich oxygen (O) atoms39, e.g., Dibenzo-18-crown-6 (DB18C6), Dibenzo-21-crown-7 (DB21C7), Dibenzo-24-crown-8 (DB24C8), and DB30C10, as depicted in Supplementary Fig. 1. Considering the ionic radius, it is crucial to select a crown ether whose cavity diameter is compatible with the cation of the perovskite40. In general, a suitable crown ether can form stable complexes with cations in perovskite, which affect the crystal growth and stability of perovskite film. Herein, we investigated the adsorption energies between the cations of WBG perovskite, which mainly contain FA (506 pm), Cs (334 pm), and Pb (238 pm), and crown ethers with different cavity diameters by means of density functional theory (DFT) calculations as shown in Supplementary Figs. 2. Mostly, the adsorption energies of crown ether and cations gradually increased as the increase in the diameter of crown ether cavity. The larger adsorption energy indicated that the spontaneous process of complexation of crown ether with cations was more readily available41. In order to select the optimum kind of crown ether modulation for WBG organic-inorganic hybridized perovskite, various crown ethers with different cavity diameters were added into the perovskite precursors, and the photovoltaic performance of the PSCs as shown in Supplementary Fig. 3 and detailed parameters in Supplementary Table 1. Notably, the crown ether molecules with different cavity diameters improved device performance compared to the control WBG PSCs, and the most remarkable improvement was obtained for DB30C10, which was attributed to its larger ring size, stronger electron-donating, and superior adsorption energies for FA+, Cs+, and Pb2+ cations with different diameters. Therefore, DB30C10 was employed as a target additive to regulate WBG PSCs for further analysis and denoted as Crown.
The uncoordinated cation defects as non-radiative recombination centers in the perovskite, and the introduction of Crown molecules can effectively promote the spontaneous complexation process. The Crown molecules form stable coordination bonds with the cations through the lone pair of electrons of the oxygen atoms of the inner cavities, and thus construct positively charged coordination sites on the molecular skeleton, which effectively attract and stabilize the negatively charged halide anions, and thus inhibit the migration of halogen ions in the WBG perovskite. At the same time, the oxygen atoms in the inner cavity of the Crown molecule can form stable interactions with the halogen anions through dipole-ion interactions, which help to balance the charge repulsion between the halogen ions and further stabilize their positions in the crystal lattice. Especially for Crown molecules containing multiple oxygen atoms, they were able to form multi-point weak interactions with the halogen ions, which not only enhance the lattice stability of the halogen ions in WBG perovskite, but also limit the migration of the halogen ions through the spatial site-barrier effect, effectively inhibiting the phase separation phenomenon. In addition, the van der Waals forces between the Crown molecules and the halogen ions in the WBG perovskite provide additional stability at short distances, and this noncovalent interaction further ensures the stability of the halogen ions in the lattice of the WBG perovskite films. Therefore, to enhance the stability of perovskite film, the incorporation of Crown into the perovskite may be effective in reducing the number of uncoordinated cation defects42, and the combination of the cation with the Crown may create a positively charged region that would be able to attract negatively charged halogen anions, thereby inhibiting the ionic migration of halogens. A hypothesis was presented in Fig. 1a that the aggregation of mixed halide anions was restrained when the cation was complexed with the Crown, resulting in a more homogeneous distribution of I and Br ions. The in situ photoluminescence (PL) mappings were performed to verify the conjecture of whether Crown would suppress the phase separation of the WBG perovskite films. As a result, the In situ time-dependent PL spectroscopy of control perovskite films during 30 min of continuous illumination with a 532 laser showed a gradual shift to the long wavelength range after 15 min as shown in Fig. 1b, which indicated that the presence of vacancy defects under continuous illumination resulted in susceptibility of mixed-halide to phase separation in the perovskite film due to massive ion migration. Moreover, the I-rich region caused a narrower bandgap while the Br-rich region induced a wider bandgap, resulting in a tendency of the photogenerated electrons and holes to migrate into the I-rich phase complex and inducing a redshift of the PL peak position. However, the PL spectra of the Crown-modified perovskite films remained stable under continuous illumination with a 532 nm laser for 30 min as shown in Fig. 1c, demonstrating that the Crown effectively inhibited the migration of halogens, reduced nonradiative recombination, and improved the stability of the films. In addition, the phases homogeneity of the perovskite film modified with Crown was significantly enhanced by the Kelvin probe force microscopy (KPFM) through comparison of Supplementary Fig. 4. Furthermore, the spectrum of the white LED lamp used for aging was continuously irradiated for 24 h in the wavelength range of 385 nm to 800 nm, and the PL mapping tests were conducted on control and Crown-modified perovskite film in a randomly selected 50 × 50 μm area using a 532 nm laser as shown in Supplementary Fig. 5. Due to the strongest illumination and sustained high-energy irradiation in the central region, the ion migration and defect aggregation of the control perovskite films were intensified, resulting in a decrease in the PL intensity of the perovskite film. However, the PL intensity of the crown-modified perovskite films showed almost no changes, indicating that Crown-modified perovskite film effectively suppressed halogen segregation and enhanced the stability of the films. Aiming to analyze the effect of Crown in a deeper molecular perspective, proton nuclear magnetic resonance (1H-NMR) spectroscopy performed in deuterated dimethyl sulfoxide (DMSO-d6) has elucidated the chemical shifts of the FA+, Cs+ and Pb2+ cations respectively upon their admixture with the Crown as shown in Fig. 1d and the detail 1H NMR spectra of control and Crown-modified perovskite film are shown in Supplementary Fig. 6, which clearly indicated that after the addition of Crown, the functional groups in Crown may form new chemical bonds or strong interactions with ions or atoms in the perovskite, causing changes in the distribution of electron clouds around these atoms, resulting in changes in the effective magnetic field they perceive and changes in chemical shifts. The hydrogen atoms located in the intra-ring of the Crown molecule possess a peculiar chemical environment43, a down-field chemical shift was observed by mixing Crown with FAI, CsI, and PbI2, respectively, which indicated that the FA+, Cs+, and Pb2+ cations integration into the ring of the Crown and formed complexes with the O atoms. In contrast, an up-field chemical shift was exhibited in the extra-ring hydrogens, suggesting that an enhancement of hydrophobicity by steric hindrance effect of the extra-ring hydrogen atoms40,44. Meanwhile, the detail FITR spectra of control and Crown-modified perovskite film, as well as the FTIR spectra of the Crown mixed with FAI, CsI, and PbI2, respectively, which also revealed the interaction of Crown with cations in WBG perovskite as shown in Supplementary Fig. 7. Moreover, the molecular binding of Crown-modified perovskite films was investigated by X-ray photoelectron spectroscopy (XPS) to demonstrate the mechanism of Crown-modified for WBG perovskite film. A conspicuous peak appeared in the O 1 s level range of 532.5 eV as shown in Supplementary Fig. 8, which suggested that the presence of Crown was playing a role in the modulation of the WBG perovskite film. Furthermore, the XPS spectra of the cations mixed with crown exhibited a downshift, implying that the interaction between the Crown and facilitating the capture of cationic defects in perovskite film as shown in Supplementary Fig. 9. However, the XPS spectra of I 3 d and Br 3 d orbitals in perovskites demonstrated a shift toward higher binding energies after modulated by the Crown as shown in Fig. 1e and f, indicating that a more stabilized energy state of halogens and inhibited the migration of the halogens. In conclusion, the mixed-halide WBG perovskites modulated by Crown can not only significantly captured the uncoordinated cation defects, but also inhibited non-radiative recombination induced by the migration of halogens, further suppressed the phase separation of WBG perovskites and enhanced the stability of the PSCs.
a Schematic diagram of halogen modulation in perovskite without and with Crown. In situ PL mapping of (b) control and (c) Crown-modified perovskite films under continuous illumination with a 532 laser. d 1H NMR spectra of the Crown in DMSO-d6 solution mixed with FAI, CsI, and PbI2, respectively, within intra-ring and extra-ring hydrogens. The XPS spectra of the (e) I 3 d orbitals and f Br 3 d orbitals obtained from the without and with Crown modified perovskite film.
Regulation of crystal growth, inhibition of defect formation and enhancement of carrier transport were the key accesses for obtaining high quality WBG PSCs45. The morphology of the perovskite films without and with Crown molecules modification was characterized by scanning electron microscopy (SEM). Figure 2a showed that the surface morphology of the film was not uniform and there was residual lead iodide (PbI2) on the surface. However, the Crown-modified perovskite films represented a homogeneous morphology as shown in Fig. 2b. Meanwhile, the cross-sectional morphology of the Crown-modified perovskite film showed that the grain boundaries were significantly reduced and the surface is flatter, as shown in Supplementary Fig. 10. To evaluate the effect of Crown on the crystallization of perovskite films, X-ray diffraction (XRD) analysis was performed as illustrated in Fig. 2c. The characteristic peak at 12.7° corresponds to PbI2 in the control perovskite film, and the residual PbI2 accelerates the photodegradation of the device to produce vacancy defects, leading to phase segregation of the I/Br phase in the mixed halide WBG perovskite. In contrast, the peak of the PbI2 disappeared completely in Crown modified perovskite films. It is noteworthy that the intensity ratio of the (100)/(110) planes increased in the Crown-modified perovskite film, implying that Crown reduced the surface energy of the (100) plane and promoted the orientation growth, and the enhanced intensity of the (111) plane by the modification with Crown may increase the stability of the perovskite film. The in situ photoluminescence (PL) spectroscopy revealed that majority of the defects in WBG perovskites were instantly formed during the rapid aggregation of clusters at the initial growth process (~30 s from the start of the spin-coating process) and ~60% of the luminescence intensity was quenched within 10 s as shown in Fig. 2d. Rapid aggregation of crystallization was responsible for rapid formation of quenching, which generated defect-rich regions during imperfect alignment of nanoparticles and led to non-radiative recombination46. However, the Crown-modified perovskite has maintained steady-state PL spectra from pre-crystallization onwards as shown in Fig. 2e.
SEM images of (a) control and (b) Crown-modified perovskite film. c XRD patterns of the perovskite films without and with Crown. In situ PL evolution of (d) control and e Crown-modified perovskite precursor ink during the spin-coating process. f TOF-SIMS depth profiling of the Crown-modified perovskite/SAM/NiOx/ITO. g Trap-filled limit voltage (VTFL) of electron-only device obtained using the space charge-limited current method. h Trap-filled limit voltage (VTFL) of hole-only device obtained using the space charge-limited current method. i TRPL spectrum of the control and Crown-modified perovskite film by a 532 nm laser from the NiOx/SAM side and from the PCBM side. (Fitting results of TRPL spectra. The effective carrier lifetime was calculated using biexponential fitting Y = A1exp(−T/T1) + A2exp(−T/T2), where A1 and A2 are the relative amplitudes, T1, T2, and Ta are the fast, slow and average carrier lifetime, respectively).
In order to determine the location of Crown in the perovskite films, we used TOF-SIMS to analyze the perovskite/SAM/NiOx/ITO structure. The I and Br ions are partially diffused into the HTL due to the relatively low migratory activation energy, leading to phase separation of I and Br ions in the perovskite film as shown in Supplementary Fig. 11. However, Crown tends to be located at the surface/interface of the film as shown in Fig. 2f, restraining the migration of I and Br ions as well as ultimately forming a more stable and uniformly distributed perovskite film. Generally, harmful ion migration and defects affect carrier transport, which was used to characterize the defect density of electrons and holes in perovskite films by space charge limited current (SCLC). The devices of ITO/SnO2/perovskite/PCBM/Ag structure tested in the dark-state showed that the VTFL of electrons was reduced from 0.85 to 0.73 V as shown in Fig. 2g, which exhibited that the electrons defect density of Crown modulation perovskite film was reduced. Meanwhile, the hole defect density tested were performed on the ITO/NiOx/SAM/perovskite/PTAA/Ag structure, and the VTFL of Crown-modified perovskite film was reduced from 0.52 to 0.28 V as shown in Fig. 2h, which indicated a reduction in the hole defect density according to the positive correlation between the density of defect states and VTFL. It is well-known that defects can have a tremendous hindering effect on the carrier transportation14. The time-resolved photoluminescence (TRPL) decay spectra of the perovskite film deposited on either a hole transport layer (HTL) or an electron transport layer (ETL) were analyzed for carrier transport without or with Crown as shown in Fig. 2i. The results demonstrated that the Crown modified perovskite film improved not only the electron extraction capability but also the hole extraction capability with the detailed parameters shown in Supplementary Table 2. In conclusion, the Crown-modified perovskite films not only suppressed the formation of defects but also enhanced the crystallinity and charge transport properties of the film, which were crucial for the development of high-performance perovskite-based solar cells.
To evaluate the effect of Crown on device performance, the inverted WBG PSCs with ITO/NiOx/Me-4PACZ/perovskite/PDAI/PCBM/BCP/Ag structures were fabricated, as illustrated in Fig. 3a. The impact of Crown concentrations on device performance was systematically optimized as shown in Supplementary Fig. 12, revealing an optimal concentration of 0.5 mg/mL for Crown-modified WBG PSCs. The photovoltaic parameters for 50 individual control and optimal Crown-modified WBG PSCs were summarized in Fig. 3b, c, demonstrating significant improvements in VOC and PCE for the Crown-modified devices. Figure 3d shows the current density-voltage (J-V) curves of the champion control and Crown-modified devices with corresponding photovoltaic parameters summarized in Supplementary Table 3. The control WBG PSC demonstrated a PCE of 19.32% (19.26%) with a VOC of 1.27 V (1.27 V), a JSC of 18.24 mA cm-2 (18.12 mA cm-2), and an FF of 82.82% (83.05%) under a reverse (forward) voltage scan. In contrast, the Crown-modified WBG PSC exhibited a PCE of 21.01% (20.95%) with a VOC of 1.30 V (1.30 V), a JSC of 18.75 mA cm–2 (18.73 mA cm–2), and an FF of 86.18% (86.01%) under a reverse (forward) voltage scan. According to Supplementary Table 4, it is currently the highest efficiency value with a bandgap of 1.77 eV. Furthermore, the integrated JSC values from the external quantum efficiency (EQE) spectra were 18.04 and 18.56 mA cm–2 for the control and Crown-modified PSCs (Fig. 3e), respectively, in accordance with the values obtained from J-V measurements. In addition, the absorbance spectrum and the bandgaps of both control and Crown-modified perovskite films were calculated to be 1.77 eV based on the first derivatives of the corresponding EQE curves as shown in Supplementary Fig. 13. Meanwhile, we extended the application of Crown modification to optimize the photovoltaic performance of FAPbI3-based NBG PSCs as shown in Supplementary Fig. 14. The Crown modification strategy not only significantly improved the efficiency of WBG PSCs, but also validated the generality of the host-guest strategy in improving the performance of NBG PSCs. Figure 3f exhibited that the corresponding control and Crown-modified devices achieved steady-state power outputs (SPO) of 19.23% and 20.94%, respectively, under constant AM 1.5 G illumination at the maximum power points (MPP) for 600 s. Comparison of the dark J-V curves revealed that the Crown-modified devices increased the shunt resistance, reduced the leakage current, and minimized the defect density as shown in Supplementary Fig. 15. The VOC increased monotonically with respect to the logarithm of the light intensity, and the ideal value (n) of 1.58 for Crown-modified PSCs was lower than that of 1.86 for the control PSCs as shown in Supplementary Fig. 16, suggesting that the Crown-modified PSCs decreased trap-assisted recombination to be consistent with the prolongation of carrier lifetimes observed in TRPL spectra. The charged complex dynamics of the control and Crown-modified PSCs were investigated by electrochemical impedance spectroscopy in Supplementary Fig. 17, and analytical results showed that the equivalent circuit fitted recombination resistance (Rrec) of the Crown-modified PSC was remarkably enhanced compared with the control device, suggesting that Crown effectively alleviated the non-radiative recombination in the perovskite and increased the VOC values of the devices. The stability was also a key parameter in evaluating the performance of the PSC. Under MPP tracking with continuous illumination in the nitrogen glovebox, the unencapsulated Crown-modified PSCs retained 95% of initial PCE after 1000 h compared with 83% for control device (Fig. 3g). The contact angle increased from 44.7° for control films to 64.96° for Crown-modified perovskite films as shown in Supplementary Fig. 18, which indicated that Crown increased the hydrophobicity of the perovskite films and effectively prevented water damage to the PSCs. Furthermore, the control and Crown modified perovskite films were observed by optical microscopy as shown in Supplementary Fig. 19, and it was revealed massive conspicuous defects on the surface of the control perovskite film after 60 min at RH = 60% ± 5%. However, the surface morphology of the Crown-modified perovskite films under the same conditions remained invariable, which indicated that the moisture stability of the Crown-modified perovskite films was improved. After 120 h of moisture stability testing at RH = 60% ± 5%, the control device suffered a significant degradation in the performance, while the Crown-modified PSCs maintained 82.2% of the initial PCE, as shown in Supplementary Fig. 20. After thermal stability test at 85 °C for 240 h, the high-temperature stability of Crown-modified WBG PSCs in dry air box can reach 91.3% of the initial efficiency, while the control device decreased to 73.2% of the initial efficiency, as shown in Supplementary Fig. 21. These results demonstrated that the incorporation of Crown in perovskite precursors significantly enhanced the overall efficiency as well as the long-term operational and humidity stability of optoelectronic devices, thereby promising a more reliable and high-performance TSCs.
a Device architecture of inverted WBG PSCs. b The Voc statistical distribution and c the PCE statistical distribution of control and Crown-modified PSCs. d J-V curves of control and Crown-modified PSCs. e EQE spectra and integrated Jsc of control and Crown-modified PSCs. f Steady-state PCE of control and Crown-modified PSCs. g Operational stability tests for control and Crown-modified PSCs measured under full solar illumination without a UV filter (light soaking under AM 1.5 G of 100 mW/cm2).
In order to advance beyond the limiting efficiency of single-junction solar cells, 1.77 eV WBG PSCs were integrated into all-perovskite TSCs. The Four-terminated (4 T) all-perovskite TSCs were prepared by mechanically stacking semi-transparent 1.77 eV WBG top cells and 1.24 eV NBG bottom cells as shown in Fig. 4a. The transmittance of the Crown-modified semi-transparent WBG PSCs was significantly superior to that of the control PSCs in the range of 900–1100 nm as shown in Fig. 4b, which was beneficial to the spectral absorption of the NBG bottom cell. The PCE of the Crown-modified semi-transparent WBG PSCs was 18.97% (Voc = 1.29 V, Jsc = 17.77 mA cm–2, and FF = 82.68%) under reverse scan, and the PCE of the filtered Sn-Pb NBG bottom cell was measured to be 9.40% (Voc = 0.82 V, Jsc = 14.80 mA cm–2, and FF = 77.14%) when the Crown-modified semi-transparent WBG PSCs were placed on the top of the Sn-Pb NBG bottom cell, resulting in a PCE of 28.37% for the 4 T TSCs as shown in Fig. 4c and detailed photovoltaic parameters in Supplementary Table 5. The EQE spectra showed that the integrated Jsc of the Crown-modified semi-transparent WBG PSCs and filtered Sn-Pb NBG bottom cell were 17.53 mA cm–2 and 12.60 mA cm–2, respectively (Fig. 4d). Under constant AM 1.5 G illumination with a MPP duration of 300 s, the Crown-modified semi-transparent WBG PSC and filtered Sn-Pb NBG bottom cell achieved SPO of 18.93% and 9.40%, respectively, while the 4 T all-perovskite TSC achieved a SPO up to 28.33% as shown in Fig. 4e. This revealed that the Crown-modified WBG perovskite top cell protected the bottom cell from the damage of intense UV radiation and minimized the thermalization loss. To efficiently minimalize the cost, we prepared two-terminal (2 T) all-perovskite TSCs using atomic layer deposition (ALD) of a 20 nm tin dioxide (SnO2) and thermal evaporation deposition of a 1 nm Au layer to form a tunnel junction as shown in Fig. 4f. The champion J-V curves of the control and Crown-modified devices, as well as the parameters of the corresponding 2 T all-perovskite TSCs as shown in Fig. 4g. In addition, the statistical data of the photovoltaic parameters based on 2 T all-perovskite TSCs as shown in Supplementary Fig. 22 and the detailed champion photovoltaic parameters in Supplementary Table 6. The results showed that the PCE of the Crown-modified 2 T all-perovskite TSCs was 28.44% (Voc = 2.14 V, Jsc = 16.36 mA cm–2, and FF = 81.31%) under reverse scan and superior to the PCE of the control device (PCE = 25.32%, Voc = 2.09 V, Jsc = 15.36 mA cm–2, and FF = 78.81%) and the certified performance of 2 T all-perovskite TSC was confirmed to be 27.92% PCE for reverse scan and 27.29% PCE for forward scan with negligible hysteresis as shown in Supplementary Fig. 23. The EQE spectra revealed a well-matched current in the top cell of the Crown-modified 1.77 eV WBG and the bottom cell of 1.24 eV Sn-Pb NBG, which contributed to the performance of the 2 T all-perovskite TSCs. These results robustly validate the effectiveness of Crown modification in 1.77 eV WBG perovskites, which contributed to a significant boost in practicality and operational efficiency within all-perovskite tandem solar cells (TSCs), thereby advancing the field of photovoltaic technology.
a Device structure of the semi-transparent 1.77 eV PSCs and NBG bottom cells for 4 T TSCs. b UV-vis transmittance spectra of semi-transparent control and Crown-modified PSCs. c J-V curves of the 4 T TSCs with Crown-modified semi-transparent 1.77 eV PSCs, Sn-Pb PSCs and filtered Sn-Pb PSCs. d EQE spectra of 4 T TSCs with semi-transparent 1.77 eV PSCs and filtered Sn-Pb PSCs. e Steady-state PCE of the 4 T TSCs with semi-transparent PSCs and filtered Sn-Pb PSCs. f Device structure of the semi-transparent 1.77 eV PSCs and NBG bottom cells for 2 T TSCs. g J-V curves of the control and Crown-modified 2 T TSCs. h EQE spectra of a 2 T TSCs with Crown-modified WBG top cell and Sn-Pb bottom cell.
In conclusion, we utilized macrocyclic Crown as additives to harmonize the coordination of halides and cations in the 1.77 eV WBG PSC. The oxygen-enriched large ether ring of Crown interacted with FA+, Cs+ and undercoordinated Pb2+, synergistically regulated the migration of the I/Br. The Crown-modified perovskite significantly suppressed I/Br segregation, reduced defect density and inhibited non-radiative recombination of photo-generated carriers. Consequently, the Crown-modified 1.77 eV PSCs achieved an excellent PCE of 21.01% and retained 95% of initial PCE after 1000 h of MPP tracing in the unencapsulated device. Moreover, the Crown-modified WBG PSCs exhibited outstanding humidity stability due to the hydrophobic exocyclic hydrogen of Crown. Additionally, the Crown-modified semi-transparent PSCs exhibited a superior transmittance in the near-infrared region and PCE up to 18.97%, and the PCE of the 4 T all-perovskite TSC achieved 28.37% after coupling with a 1.24 Sn-Pb perovskite bottom cell. Furthermore, the PCE of Crown-modified 2 T all-perovskite TSC yielded 28.44% (certified 27.92%). This study provided a reference for the design of a host-guest strategy to modify efficient and stable WBG PSCs and TSCs.
Nickel oxide (NiOx) nanoparticles (NPs) were synthesized according to previous work47. [4-(3,6-Dimethyl-9H-carbazol-9-yl)butyl] phosphonic acid (Me-4PACz), 1,3 propyldiammonium diiodide (PDAI2), ethane-1,2-diammonium iodide (EDAI2), bathocuproine (BCP) and Poly(3,4-ethylenedioxythiophene): poly(styrene sulfonate) (PEDOT:PSS) aqueous solution were purchased from Xi’an Polymer Light Technology Corp. 4,4′,4″-nitrilotribenzoic acid (NA) was purchased from Aladdin Biochemical Technology. Cesium iodide (CsI), lead iodide (PbI2, 99.999%), lead bromide (PbBr2, ≥98%), lead chloride (PbCl2, 99.99%), methylammonium iodide (MAI), tin(II) fluoride (SnF2), tin(II) iodide (SnI2), glycine hydrochloride (GlyHCl) and ammonium thiocyanate (NH4SCN) were purchased from Advanced Election Technology Co., Ltd. Dimethylammonium iodide (DMAI) and formamidinium iodide (FAI) were purchased from Greatcell Solar. [6,6]-phenyl-C61-butyric acid methyl ester (PC61BM, >99.5%) were purchased from Nano-C. Dibenzo-18-crown-6 (DB18C6), Dibenzo-21-crown-7 (DB21C7), Dibenzo-24-crown-8 (DB24C8), Dibenzo-30-crown-10 (DB30C10) and Aluminum-doped zinc oxide (AZO) nanoparticle ink (N-21X, 2.5 wt% Al:ZnO, work function: 3.9 eV) were purchased from Sigma-Aldrich. Precursors of tetrakis (dimethylamino) tin (IV) (99.9999%, Nanjing Ai Mou Yuan Scientific Equipment). IZO sputtering target was purchased from Zhongsheng Hengan. All solvents were purchased from Sigma-Aldrich. All the solvents and reagents were purchased and used directly without further purification.
1.4 mol L-1 of Cs0.3FA0.6DMA0.1Pb(I0.7Br0.3)3 1.77 eV-bandgap perovskite precursor solutions were prepared by dissolving DMAI (0.14 M), CsI (0.42 M), FAI (0.84 M), PbCl2 (0.028 M), PbBr2 (0.63 M) and PbI2 (0.77 M) in pure Dimethyl sulfoxide (DMSO) solvent to dissolve completely. The 1 mL of precursor solution was added with x mg DB30C10 solute (x = 0.3, 0.5, 1.0 and 2.0). Then the perovskite precursor solutions were stirred overnight in a nitrogen-filled glovebox and used without any further treatment.
The pre-patterned ITO substrates (Advanced Election Technology Co., Ltd, 15 Ω sq−1) were cleaned and treated with UV-ozone for 20 min. The 10 mg ml–1 NiOx NP aqueous ink onto ITO substrates at 4000 r.p.m. for 30 s and annealed at 100 °C for 10 min under ambient conditions. Then, the obtained NiOx films were immediately transferred into a nitrogen-filled glovebox. A self-assembled monolayer of mixed-solution Me-4PACz and NA (1 mM in ethanol, volume ratio 3:1) at 4000 r.p.m. for 30 s, followed by 10 min of annealing at 100 °C. The perovskite absorber layers were deposited in the N2-filled glove box with controlled H2O and O2 levels below 0.1 ppm, and the temperature was monitored to be 23 °C. 50 µL of perovskite precursor was dropped onto the HTL substrate. The substrate was spun at 2000 r.p.m. for 15 s with an acceleration of 1000 r.p.m. s-1 at first, and then at 4000 r.p.m. for the 45 s with an acceleration of 2000 r.p.m. s-1. the nitrogen gun was vertically positioned 5 cm above the top of the substrates and the gas flow started after 30 s of the spin and duration of 20 s when the gas flow pressure was 30 psi. Subsequently, the wet-films were annealed at 100 °C for 30 min. The 2 mg ml-1 of PDAI2 solution in IPA was spin coated onto the perovskite surface at 4,000 rpm for 30 s and annealed at 100 °C for 5 min. The 23 mg ml–1 of PC61BM solution in CB was spin-coated at 2,500 r.p.m. for 40 s and then annealed at 70 °C for 10 min. Then, 0.5 mg BCP was added into 1 mL IPA and was spin-coated on PC61BM film at 5000 r.p.m. for 30 s. Finally, a 100 nm Ag electrode with an active area of 0.1017 cm2 was deposited by thermal evaporation.
The semi-transparent PSCs were prepared by spin-coating the AZO solution (2.5 wt% AZO nanoparticle solution: IPA = 3:20 by volume) onto the PCBM film surface at 2000 r.p.m. for 30 s and then annealed at 70 °C for 10 min. Thereafter, 20 nm of SnOx layer were deposited on top of the AZO film at 100 °C in an ALD reactor (MNT-S100-L4S1, Jiangsu MNT Micro and Nanotech Co., LTD.). Each ALD cycle consists of a H2O vapor dose of 0.02 s, followed by a purge of 25 s, then a TDMA dose of 0.2 s, followed by a purge of 20 s. 100 nm IZO electrode was sputtered in TRP450 system with a processing pressure of 0.5 Pa, sputtering power was100 W and the gas flow was 30 sccm of argon gas and 100 nm of Ag grids were prepared around the IZO film.
1.24 eV bandgap Cs0.1FA0.6MA0.3Sn0.5Pb0.5I3 perovskite films, 1.8 M perovskite precursor solution was prepared by dissolving 46.8 mg CsI, 85.8 mg MAI, 185.7 mg FAI, 14.1 mg SnF2, 335.3 mg SnI2, 414.9 mg PbI2, 4.0 mg glycine hydrochloride and 2.7 mg NH4SCN in mixed solvents of 0.25 mL DMSO and 0.75 mL DMF solvent. Then, the perovskite precursors were stirred at 65 °C for 12 h and filtered using a 0.22 μm PTFE membrane before use.
The pre-patterned ITO substrates (Advanced Election Technology Co., Ltd, 15 Ω sq−1) were cleaned and treated with UV-ozone for 30 min. The PEDOT:PSS solution was spin-coated on the top of ITO with 500 r.p.m. for 10 s and 4000 r.p.m. for 30 s, followed by annealing at 140 °C for 20 min in air and annealing at 140 °C for 30 min in glove box. The Sn-Pb perovskite was spun at 1000 r.p.m. for 10 s with an acceleration of 200 r.p.m. s–1 at first, and then at 4000 r.p.m. for the 40 s with an acceleration of 1000 r.p.m. s–1. Room temperature chlorobenzene (400 μL) was used as the antisolvent. The chlorobenzene was quickly dripped onto the surface of the spinning substrate over an interval of 1 s during the second spin coating step at 20 s before the end of the procedure. The substrate was then immediately annealed on a 100 °C hot plate for 10 min, followed by annealing at 65 °C for over 10 min. The 1.0 mg/ml EDAI2 in IPA solution was spin-coated on the perovskite film with 4000 r.p.m. for 30 s and annealing at 100 °C for 5 min. The 23 mg ml–1 of PC61BM solution in CB was spin-coated at 2500 r.p.m. for 40 s and then annealed at 70 °C for 10 min. Then, 0.5 mg BCP was added into 1 mL IPA and was spin-coated on PC61BM film at 5000 r.p.m. for 30 s. Finally, the Ag electrode (100 nm) was deposited through shadow mask under a pressure of 5 × 10−4 Pa.
The fabrication of WBG PSCs was completed as described above up to the deposition of 20 nm of ALD-SnO2. Subsequently, 1 nm of Au was deposited by thermal evaporation. Next, the PEDOT:PSS solution was spin-coated on the top of ITO with 500 r.p.m. for 10 s and 4000 r.p.m. for 30 s, followed by annealing at 140 °C for 20 min in air and annealing at 140 °C for 30 min in glove box. Subsequently, the fabrication of NGB PSCs was carried out in an N2-filled a glove box.
All the data supporting the findings of this study are available within this article and its Supplementary Information. Any additional information can be obtained from corresponding authors upon request. Source data are provided with this paper.
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This work was supported by the National Natural Science Foundation of China (No. 52302229; No. 52302333), the State Key Laboratory of Photovoltaic Science and Technology of China (No. 202401030301), Guangdong Basic and Applied Basic Research Foundation (2023A1515012788) and Shenzhen Science and Technology Program (KQTD20221101093647058, ZDSYS20210706144000003).
These authors contributed equally: Xinxin Lian, Mingjing Jin.
State Key Laboratory of Photovoltaic Science and Technology, Institute of Optoelectronics, College of Future Information Technology, Fudan University, Shanghai, China
Xinxin Lian, Ming Luo, Ying Hu, Zhijie Wang, Haiyun Li, Chunyu Xu, Dongrui Jiang, Yifan Chen, Hong Zhang, Xiaoliang Mo & Junhao Chu
Shanghai Frontiers Science Research Base of Intelligent Optoelectronics and Perception, Fudan University, Shanghai, China
Xinxin Lian, Ming Luo, Ying Hu, Zhijie Wang, Haiyun Li, Chunyu Xu, Dongrui Jiang, Yifan Chen, Hong Zhang, Xiaoliang Mo & Junhao Chu
Yiwu Research Institute of Fudan University, Yiwu, China
Xinxin Lian, Hong Zhang, Xiaoliang Mo & Junhao Chu
Faculty of Materials Science and Energy Engineering, Shenzhen University of Advanced Technology (SUAT), Shenzhen, China
Mingjing Jin, Weideren Dai & Yang Bai
Institute of Technology for Carbon Neutrality, Shenzhen Institutes of Advanced Technology (SIAT), Chinese Academy of Sciences, Shenzhen, China
Mingjing Jin & Yang Bai
School of Materials Science and Engineering, Hubei University, Wuhan, China
Weideren Dai
State Key Laboratory for Mechanical Behavior of Materials, Xi’an Jiaotong University, Xi’an, Shaanxi, China
Yuanjiang Lv & Fei Ma
Key Laboratory of Flexible Electronics (KLOFE), Institute of Advanced Materials (IAM), Nanjing Tech University, Nanjing, China
Hao Min & Jin Chang
Graduate Institute of Energy and Sustainability Tech, National Taiwan, University of Science and Technology, Taipei City, Taiwan
Tzu-Sen Su
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H.Z., X.L.M., and J.H.C. supervised the project. H.Z. and X.X.L. convinced the idea. X.X.L. fabricated the WBG PSCs and conducted most of the characterizations. M.J.J., W.D. and Y.B. contributed to the fabrication and characterization of 2 T TSCs. Y.J.L. and F.M. were responsible for the DFT simulation. H.M. and J.C. were responsible for the in situ PL/UV-vis characterizations of WBG perovskite film formation. Y.H were responsible for the SEM and M.L., Z.J.W., H.Y.L., D.R.J., C.Y.X., T.S.S., and Y.F.C. were participated in the optimization of WBG PSCs. X.X.L. wrote the first draft, H.Z. revised the manuscript. All authors contributed to the proofs of the manuscript.
Correspondence to Yang Bai, Hong Zhang or Xiaoliang Mo.
The authors declare no competing interests.
Nature Communications thanks Peter Chen, 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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Lian, X., Jin, M., Dai, W. et al. A supramolecular approach to improve the performance and operational stability of all-perovskite tandem solar cells. Nat Commun 16, 7173 (2025). https://doi.org/10.1038/s41467-025-62391-9
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