Abstract
Two-dimensional Ruddlesden–Popper layered metal-halide perovskites have attracted increasing attention for their desirable optoelectronic properties and improved stability compared to their three-dimensional counterparts. However, such perovskites typically consist of multiple quantum wells with a random well width distribution. Here, we report phase-pure quantum wells with a single well width by introducing molten salt spacer n-butylamine acetate, instead of the traditional halide spacer n-butylamine iodide. Due to the strong ionic coordination between n-butylamine acetate and the perovskite framework, a gel of a uniformly distributed intermediate phase can be formed. This allows phase-pure quantum well films with microscale vertically aligned grains to crystallize from their respective intermediate phases. The resultant solar cells achieve a power conversion efficiency of 16.25% and a high open voltage of 1.31 V. After keeping them in 65 ± 10% humidity for 4,680 h, under operation at 85 °C for 558 h, or continuous light illumination for 1,100 h, the cells show <10% efficiency degradation.
This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 digital issues and online access to articles
$119.00 per year
only $9.92 per issue
Rent or buy this article
Prices vary by article type
from$1.95
to$39.95
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
Data availability
The datasets generated and/or analysed during the current study are available within the paper and its Supplementary Information. Source data are provided with this paper.
Code availability
Any applicable code relevant to the findings is available from the authors upon reasonable request.
References
Quintero-Bermudez, R. et al. Compositional and orientational control in metal halide perovskites of reduced dimensionality. Nat. Mater. 17, 900–907 (2018).
Zhou, N. et al. Exploration of crystallization kinetics in quasi two-dimensional perovskite and high performance solar cells. J. Am. Chem. Soc. 140, 459–465 (2017).
Yuan, M. et al. Perovskite energy funnels for efficient light-emitting diodes. Nat. Nanotechnol. 11, 872–877 (2016).
Blancon, J.-C. et al. Scaling law for excitons in 2D perovskite quantum wells. Nat. Commun. 9, 2254 (2018).
Lin, Y. et al. Unveiling the operation mechanism of layered perovskite solar cells. Nat. Commun. 10, 1008 (2019).
Quan, L. et al. Ligand-stabilized reduced-dimensionality perovskites. J. Am. Chem. Soc. 138, 2649–2655 (2016).
Tsai, H. et al. Design principles for electronic charge transport in solution-processed vertically stacked 2D perovskite quantum wells. Nat. Commun. 9, 2130 (2018).
Tsai, H. et al. High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells. Nature 536, 312–316 (2016).
Yan, K. et al. Hybrid halide perovskite solar cell precursors: colloidal chemistry and coordination engineering behind device processing for high efficiency. J. Am. Chem. Soc. 137, 4460–4468 (2015).
McMeekin, D. P. et al. Crystallization kinetics and morphology control of formamidinium-cesium mixed-cation lead mixed-halide perovskite via tunability of the colloidal precursor solution. Adv. Mater. 29, 1607039 (2017).
Dou, L. et al. Atomically thin two-dimensional organic-inorganic hybrid perovskites. Science 349, 1518–1521 (2015).
Cao, D. et al. 2D homologous perovskites as light-absorbing materials for solar cell applications. J. Am. Chem. Soc. 137, 7843–7850 (2015).
Soe, C. M. M. et al. Understanding film formation morphology and orientation in high member 2D Ruddlesden–Popper perovskites for high-efficiency solar cells. Adv. Energy Mater. 8, 1700979 (2018).
Qing, J. et al. Aligned and graded type-II Ruddlesden-Popper perovskite films for efficient solar cells. Adv. Energy Mater. 8, 1800185 (2018).
Shang, Y. et al. Highly stable hybrid perovskite light-emitting diodes based on Dion-Jacobson structure. Sci. Adv. 5, eaaw8072 (2019).
Proppe, A. et al. Synthetic control over quantum well width distribution and carrier migration in low-dimensional perovskite photovoltaics. J. Am. Chem. Soc. 140, 2890–2896 (2018).
Liu, J. et al. Observation of internal photoinduced electron and hole separation in hybrid two-dimensional perovskite films. J. Am. Chem. Soc. 139, 1432–1435 (2017).
Liang, Y. et al. Lasing from mechanically exfoliated 2D homologous Ruddlesden–Popper perovskite engineered by inorganic layer thickness. Adv. Mater. 39, 1903030 (2019).
Wang, N. et al. Perovskite light-emitting diodes based on solution-processed self-organized multiple quantum wells. Nat. Photon. 10, 699–704 (2016).
Yantara, N. et al. Designing efficient energy funneling kinetics in Ruddlesden–Popper perovskites for high-performance light-emitting diodes. Adv. Mater. 30, 1800818 (2018).
Byun, J. et al. Efficient visible quasi-2D perovskite light-emitting diodes. Adv. Mater. 28, 7515–7520 (2016).
Xing, G. et al. Transcending the slow bimolecular recombination in lead-halide perovskites for electroluminescence. Nat. Commun. 8, 14558 (2017).
Blancon, J.-C. et al. Extremely efficient internal exciton dissociation through edge states in layered 2D perovskites. Science 355, 1288–1292 (2017).
Zhang, X. et al. Phase transition control for high performance Ruddlesden–Popper perovskite solar cells. Adv. Mater. 30, 1707166 (2018).
Chao, L. et al. Room-temperature molten salt for facile fabrication of efficient and stable perovskite solar cells in ambient air. Chem 5, 995–1006 (2019).
Xia, Y. et al. Management of perovskite intermediates for highly efficient inverted planar heterojunction perovskite solar cells. J. Mater. Chem. A 5, 3193–3202 (2017).
Li, L. et al. The additive coordination effect on hybrids perovskite crystallization and high-performance solar cell. Adv. Mater. 28, 9862–9868 (2016).
Bi, D. et al. Polymer-templated nucleation and crystal growth of perovskite films for solar cells with efficiency greater than 21%. Nat. Energy 1, 16142 (2016).
Liu, Y. et al. Ultrahydrophobic 3D/2D fluoroarene bilayer-based water-resistant perovskite solar cells with efficiencies exceeding 22%. Sci. Adv. 5, eaaw2543 (2019).
Chen, P. et al. In situ growth of 2D perovskite capping layer for stable and efficient perovskite solar cells. Adv. Funct. Mater. 28, 1706923 (2018).
Ono, L. K. et al. Progress toward stable lead halide perovskite solar cells. Joule 2, 1961–1990 (2018).
Spanopoulos, I. et al. Uniaxial expansion of the 2D Ruddlesden−Popper perovskite family for improved environmental stability. J. Am. Chem. Soc. 141, 5518–5534 (2019).
Okamoto, K. et al. Surface-plasmon-enhanced light emitters based on InGaN quantum wells. Nat. Mater. 3, 601–605 (2004).
Ravel, B. et al. Athena, Artemis, Hephaestus: data analysis for X-ray absorption spectroscopy using IFEFFIT. J. Synchrotron Rad. 12, 537–541 (2005).
Nahringbauer, I. et al. Hydrogen bond studies. XIV. The crystal structure of ammonium acetate. Acta Cryst. 23, 956–965 (1967).
Acknowledgements
This work was financially supported by the Natural Science Foundation of China (51972172, 61705102, 61605073, 61935017, 91833304 and 91733302), the National Key R&D Program of China (2017YFB1002900, 2017YFA0403400), the Macau Science and Technology Development Fund (FDCT-116/2016/A3, FDCT-091/2017/A2 and FDCT-014/2017/AMJ), the University of Macau (SRG2016-00087-FST and MYRG2018-00148-IAPME), Natural Science Foundation of Guangdong Province, China (2019A1515012186), Projects of International Cooperation and Exchanges NSFC (51811530018), Young 1000 Talents Global Recruitment Program of China, Jiangsu Specially-Appointed Professors Program and ‘Six Talent Peaks’ Project in Jiangsu Province, China.
Author information
Authors and Affiliations
Contributions
Y.C. and G.X. conceived the idea and designed the experiments. Y.C., G.X. and W.H. supervised the work. C.L., H.G. and Y.X. carried out the device fabrication and characterizations. X.L., L.C., T.N. and B.L. also contributed to device fabrication. C.L., H.G., H.D., H.Y. and S.C. conducted the optical spectra measurements. H.G., M.F. and H.L. synthesized the BAAc. J.Z., S.Z. and H.G. conducted the X-ray absorption fine structure spectroscopy measurements and analysed the data. Y.P., Y.H. and H.G. carried out the scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy mappings. Z.W., J.X. and X.R. carried out the density functional theory calculations. GIWAXS was performed and analysed by W.H., L.S. and X.G., supported by the BL14B1 beamline of the Shanghai Synchrotron Radiation Facility. C.L., H.G. and Y.X. wrote the first draught of the manuscript. Y.C., Y.X., G.X., J.W., G.S. and W.H. participated in data analysis and provided major revisions. All authors discussed the results and commented on the manuscript.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Note 1, Figs. 1–14, Tables 1–5 and references.
Supplementary Data 1
Numerical data used to generate Supplementary Fig. 14.
Source data
Source Data Fig. 1
Numerical data used to generate Fig. 1.
Source Data Fig. 2
Numerical data used to generate Fig. 2.
Source Data Fig. 3
Numerical data used to generate Fig. 3.
Source Data Fig. 4
Numerical data used to generate Fig. 4.
Rights and permissions
About this article
Cite this article
Liang, C., Gu, H., Xia, Y. et al. Two-dimensional Ruddlesden–Popper layered perovskite solar cells based on phase-pure thin films. Nat Energy 6, 38–45 (2021). https://doi.org/10.1038/s41560-020-00721-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41560-020-00721-5
This article is cited by
-
High-efficiency reinforcement learning with hybrid architecture photonic integrated circuit
Nature Communications (2024)
-
Frequency-selective perovskite photodetector for anti-interference optical communications
Nature Communications (2024)
-
Phase dimensions resolving of efficient and stable perovskite light-emitting diodes at high brightness
Nature Photonics (2024)
-
Inverted perovskite solar cells with over 2,000 h operational stability at 85 °C using fixed charge passivation
Nature Energy (2023)
-
Phase-pure two-dimensional layered perovskite thin films
Nature Reviews Materials (2023)