Picosecond energy transfer and multiexciton transfer outpaces auger recombination in binary cdse nanoplatelet solids

ABSTRACT Fluorescence resonance energy transfer (FRET) enables photosynthetic light harvesting1, wavelength downconversion in light-emitting diodes2 (LEDs), and optical biosensing schemes3.

The rate and efficiency of this donor to acceptor transfer of excitation between chromophores dictates the utility of FRET and can unlock new device operation motifs including quantum-funnel

solar cells4, non-contact chromophore pumping from a proximal LED5, and markedly reduced gain thresholds6. However, the fastest reported FRET time constants involving spherical quantum dots

(0.12–1 ns; refs 7, 8, 9) do not outpace biexciton Auger recombination (0.01–0.1 ns; ref. 10), which impedes multiexciton-driven applications including electrically pumped lasers11 and

carrier-multiplication-enhanced photovoltaics12,13. Few-monolayer-thick semiconductor nanoplatelets (NPLs) with tens-of-nanometre lateral dimensions14 exhibit intense optical transitions14

and hundreds-of-picosecond Auger recombination15,16, but heretofore lack FRET characterizations. We examine binary CdSe NPL solids and show that interplate FRET (∼6–23 ps, presumably for

co-facial arrangements) can occur 15–50 times faster than Auger recombination15,16 and demonstrate multiexcitonic FRET, making such materials ideal candidates for advanced technologies.

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  Download references ACKNOWLEDGEMENTS This work was performed, in part, at the Center for Nanoscale Materials, a US Department of Energy, Office of Science, Office of Basic Energy Sciences

User Facility under Contract No. DE-AC02-06CH11357. C.E.R. acknowledges support by a National Science Foundation Graduate Research Fellowship under Grant No. DGE-0824162. D.V.T. acknowledges

support by the NSF MRSEC Program under Award Number DMR 14-20709 and thanks the II-VI Foundation and Keck Foundation. H.Z. and A.O.G. acknowledge support by the US Army Research Office

under grant number W911NF-12-1-0407 and the Volkswagen Foundation (Germany). AUTHOR INFORMATION AUTHORS AND AFFILIATIONS * Department of Chemistry, Northwestern University, Evanston,

Illinois 60208, USA Clare E. Rowland & Richard D. Schaller * Department of Chemistry and James Franck Institute, University of Chicago, Chicago, Illinois 60637, USA Igor Fedin & 

Dmitri V. Talapin * Department of Physics and Astronomy, Ohio University, Athens, Ohio 45701, USA Hui Zhang & Alexander O. Govorov * Center for Nanoscale Materials, Argonne National

Laboratory, Argonne, Illinois 60439, USA Stephen K. Gray, Dmitri V. Talapin & Richard D. Schaller Authors * Clare E. Rowland View author publications You can also search for this author

inPubMed Google Scholar * Igor Fedin View author publications You can also search for this author inPubMed Google Scholar * Hui Zhang View author publications You can also search for this

author inPubMed Google Scholar * Stephen K. Gray View author publications You can also search for this author inPubMed Google Scholar * Alexander O. Govorov View author publications You can

also search for this author inPubMed Google Scholar * Dmitri V. Talapin View author publications You can also search for this author inPubMed Google Scholar * Richard D. Schaller View author

publications You can also search for this author inPubMed Google Scholar CONTRIBUTIONS Sample synthesis and electron microscopy were performed by I.F. and D.V.T. Optical measurements and

data analysis were performed by C.E.R. and R.D.S. Computational work was performed by H.Z., A.O.G. and S.K.G. All authors contributed to the writing of the manuscript. CORRESPONDING AUTHOR

Correspondence to Richard D. Schaller. ETHICS DECLARATIONS COMPETING INTERESTS The authors declare no competing financial interests. SUPPLEMENTARY INFORMATION SUPPLEMENTARY INFORMATION

Supplementary Information (PDF 846 kb) RIGHTS AND PERMISSIONS Reprints and permissions ABOUT THIS ARTICLE CITE THIS ARTICLE Rowland, C., Fedin, I., Zhang, H. _et al._ Picosecond energy

transfer and multiexciton transfer outpaces Auger recombination in binary CdSe nanoplatelet solids. _Nature Mater_ 14, 484–489 (2015). https://doi.org/10.1038/nmat4231 Download citation *

Received: 08 August 2014 * Accepted: 29 January 2015 * Published: 16 March 2015 * Issue Date: May 2015 * DOI: https://doi.org/10.1038/nmat4231 SHARE THIS ARTICLE Anyone you share the

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