Journal
NATURE CHEMISTRY
Volume 5, Issue 7, Pages 602-606Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NCHEM.1654
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Funding
- US Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering [DE-FG02-07ER46454]
- National Institutes of Health through the MIT Laser Biomedical Resource Center [P41EB015871-26A1]
- National Science Foundation Graduate Research Fellowship Program
- Fannie and John Hertz Foundation
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The spectral linewidth of an ensemble of fluorescent emitters is dictated by the combination of single-emitter linewidths and sample inhomogeneity. For semiconductor nanocrystals, efforts to tune ensemble linewidths for optical applications have focused primarily on eliminating sample inhomogeneities, because conventional single-molecule methods cannot reliably build accurate ensemble-level statistics for single-particle linewidths. Photon-correlation Fourier spectroscopy in solution (S-PCFS) offers a unique approach to investigating single-nanocrystal spectra with large sample statistics and high signal-to-noise ratios, without user selection bias and at fast timescales. With S-PCFS, we directly and quantitatively deconstruct the ensemble linewidth into contributions from the average single-particle linewidth and from sample inhomogeneity. We demonstrate that single-particle linewidths vary significantly from batch to batch and can be synthetically controlled. These findings delineate the synthetic challenges facing underdeveloped nanomaterials such as InP and InAs core-shell particles and introduce new avenues for the synthetic optimization of fluorescent nanoparticles.
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