Interface Molecular Engineering for Laminated Monolithic Perovskite/Silicon Tandem Solar Cells with 80.4% Fill Factor

César Omar Ramírez Quiroz, George D. Spyropoulos, Michael Salvador, Loïc M. Roch, Marvin Berlinghof, José Darío Perea, Karen Forberich, Laura Isabelle Dion-Bertrand, Nadine J. Schrenker, Andrej Classen, Nicola Gasparini, Ganna Chistiakova, Mathias Mews, Lars Korte, Bernd Rech, Ning Li, Frank Hauke, Erdmann Spiecker, Tayebeh Ameri, Steve AlbrechtGonzalo Abellán, Salvador León, Tobias Unruh, Andreas Hirsch, Alán Aspuru-Guzik, Christoph J. Brabec

Research output: Contribution to journalArticlepeer-review

39 Scopus citations


A multipurpose interconnection layer based on poly(3,4-ethylenedioxythiophene) doped with poly(styrene sulfonate) (PEDOT:PSS), and d-sorbitol for monolithic perovskite/silicon tandem solar cells is introduced. The interconnection of independently processed silicon and perovskite subcells is a simple add-on lamination step, alleviating common fabrication complexities of tandem devices. It is demonstrated experimentally and theoretically that PEDOT:PSS is an ideal building block for manipulating the mechanical and electrical functionality of the charge recombination layer by controlling the microstructure on the nano- and mesoscale. It is elucidated that the optimal functionality of the recombination layer relies on a gradient in the d-sorbitol dopant distribution that modulates the orientation of PEDOT across the PEDOT:PSS film. Using this modified PEDOT:PSS composite, a monolithic two-terminal perovskite/silicon tandem solar cell with a steady-state efficiency of 21.0%, a fill factor of 80.4%, and negligible open circuit voltage losses compared to single-junction devices is shown. The versatility of this approach is further validated by presenting a laminated two-terminal monolithic perovskite/organic tandem solar cell with 11.7% power conversion efficiency. It is envisioned that this lamination concept can be applied for the pairing of multiple photovoltaic and other thin film technologies, creating a universal platform that facilitates mass production of tandem devices with high efficiency.
Original languageEnglish (US)
Pages (from-to)1901476
JournalAdvanced Functional Materials
Issue number40
StatePublished - Aug 7 2019

Bibliographical note

KAUST Repository Item: Exported on 2020-10-01
Acknowledgements: The Cluster of Excellence funded this work through “Engineering of Advanced Materials” (EAM). The authors acknowledge financial support from the DFG research-training group GRK 1896 at Erlangen University and from the Joint Project Helmholtz-Institute Erlangen Nürnberg (HI-ERN) under Project No. DBF01253, respectively. C.J.B. acknowledges the financial support through the “Aufbruch Bayern” initiative of the state of Bavaria (EnCN and Solar Factory of the Future) and the “Solar Factory of the Future” with the Energy Campus Nürnberg (EnCN). S.L. acknowledges the Real Colegio Complutense in Harvard for a research grant, and to the Spanish Ministerio de Ciencia e Innovación for a fellowship through the Salvador de Madariaga Program. L.M.R. and A.A.-G. acknowledge support from Tata Sons Limited – Alliance Agreement (A32391). The computations in this paper were done on the Odyssey cluster supported by the FAS Division of Science, Research Computing Group at Harvard University, and on the Arran cluster supported by the Health Sciences Platform (HSP) at Tianjin University. C.O.R.Q. would like to acknowledge M. Möhrensen for his assistance in graphic design. Similarly, C.O.R.Q. would like to acknowledge Gebhard Matt and Ievgen Levchuk for helpful discussion. G.A. thanks support by the European Research Council (ERC Starting Grant 804110), the Spanish MINECO through the Excellence Unit María de Maeztu (MDM-2015-0538), the Generalitat Valenciana (CIDEGENT/2018/001), and the Deutsche Forschungsgemeinschaft (DFG; FLAG-ERA AB694/2-1). G.A. would like to acknowledge Vicent Lloret for his assistance with the experimental work. B. R., L.K., S.A., and G.C. acknowledge support from BMWi through the “PersiST” project (Grant No. 0324037C). S.A. acknowledges funding by the BMBF within the project “Materialforschung für die Energiewende” for his Young Investigator Group (Grant No. 03SF0540). T.A. gratefully acknowledges the financial support of the Solar Technologies go Hybrid (SolTech) and Bavarian Equal Opportunities Sponsorship – Förderung von Frauen in Forschung und Lehre (FFL). T.U. and M.B. gratefully acknowledge the funding of the German Federal Ministry of Education and Research (BMBF, Project No. 05K16WEB). C.O.R.Q. would like to gratefully acknowledge the financial support from The Mexican National Council for Science and Technology (CONACYT). C.O.R.Q. wrote the manuscript with comments from all coauthors and highlighted contributions from M.S. C.O.R.Q. coordinated and performed photovoltaic device fabrication. C.O.R.Q. coordinated all experiments, measurements, and simulations. G.D.S. assisted with the tandem lamination process. C.O.R.Q. and K.F. performed optical simulations. M.S., G.D.S., N.L., T.A., and A.A.-G. assisted with data interpretation, story layout design, and contributed ideas. C.O.R.Q., N.S., and E.S. contributed with the electron microscopy analysis. C.O.R.Q., M.B., and T.B. contributed with X-ray studies. C.O.R.Q., G.A., F.H., and A.H. contributed with Raman studies. L.-I.D.-B., and N.G. assisted with PL measurements. N.G. and A.C. assisted with FTPS and PL data analysis and interpretation. M.M., G.C., L.K., B.R., and S.A. provided silicon cells. QM/DFT calculations and analysis were performed by L.M.R. MD parametrization was done by S.L., and MD simulations were performed and analyzed by S.L. and J.D.P. C.J.B. supervised the project.


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