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Open Access Green as soon as Postprint is submitted to ZB.
Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths.
Nat. Chem. 5, 602-606 (2013)
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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Publication type
Article: Journal article
Document type
Scientific Article
ISSN (print) / ISBN
1755-4330
e-ISSN
1755-4349
Journal
Nature chemistry
Quellenangaben
Volume: 5,
Issue: 7,
Pages: 602-606
Publisher
Nature Publishing Group
Publishing Place
London
Non-patent literature
Publications
Reviewing status
Peer reviewed
Institute(s)
Helmholtz Pioneer Campus (HPC)