Probing Linewidths and Biexciton Quantum Yields of Single Cesium Lead Halide Nanocrystals in Solution

Utzat, Hendrik; Shulenberger, Katherine E.; Achorn, Odin B.; Nasilowski, Michel; Sinclair, Timothy S.; Bawendi, Moungi G.

doi:10.1021/acs.nanolett.7b03120

Title: Probing Linewidths and Biexciton Quantum Yields of Single Cesium Lead Halide Nanocrystals in Solution

Journal Article · 17 October 2017 · Nano Letters

DOI: https://doi.org/10.1021/acs.nanolett.7b03120 · OSTI ID:1470544

Utzat, Hendrik ^[1]; Shulenberger, Katherine E. ^[1]; Achorn, Odin B. ^[1]; Nasilowski, Michel ^[1]; Sinclair, Timothy S. ^[1];

^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry

Cesium lead halide (CsPbX₃, X = Cl, Br, I) perovskite nanocrystals (PNCs) have recently become a promising material for optoelectronic applications due to their high emission quantum yields and facile band gap tunability via both halide composition and size. The spectroscopy of single PNCs enhances our understanding of the effect of confinement on excitations in PNCs in the absence of obfuscating ensemble averaging and can also inform synthetic efforts. However, single PNC studies have been hampered by poor PNC photostability under confocal excitation, precluding interrogation of all but the most stable PNCs, and leading to a lack of understanding of PNCs in the regime of high confinement. Here, we report the first comprehensive spectroscopic investigation of single PNC properties using solution-phase photon-correlation methods, including both highly confined and blue-emitting PNCs, previously inaccessible to single NC techniques. With minimally perturbative solution-phase photon-correlation Fourier spectroscopy (s-PCFS), we establish that the ensemble emission linewidth of PNCs of all sizes and compositions is predominantly determined by the intrinsic single PNC linewidth (homogeneous broadening). The single PNC linewidth, in turn, dramatically increases with increasing confinement, consistent with what has been found for II–VI semiconductor nanocrystals. With solution-phase photon antibunching measurements, we survey the biexciton-to-exciton quantum yield ratio (BX/X QY) in the absence of user-selection bias or photodegradation. Remarkably, the BX/X QY ratio depends both on the PNC size and halide composition, with values between ~2% for highly confined bromide PNCs and ~50% for intermediately confined iodide PNCs. Our results suggest a wide range of underlying Auger rates, likely due to transitory charge carrier separation in PNCs with relaxed confinement.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001088

OSTI ID:: 1470544

Journal Information:: Nano Letters, Vol. 17, Issue 11; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; ISSN 1530-6984

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
77 NANOSCIENCE AND NANOTECHNOLOGY
Cesium lead halide perovskites
perovskite nanocrystals
biexciton quantum yield
spectral lineshapes
single nanocrystal spectroscopy
photon correlation Fourier spectroscopy
semiconductor nanocrystals
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Title: Probing Linewidths and Biexciton Quantum Yields of Single Cesium Lead Halide Nanocrystals in Solution

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