PuSH - Publication Server of Helmholtz Zentrum München: Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths.

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Cui, J. ; Beyler, A.P.* ; Marshall, L.F.* ; Chen, O.* ; Harris, D.K.* ; Wanger, D.D.* ; Brokmann, X.* ; Bawendi, M.G.*

Direct probe of spectral inhomogeneity reveals synthetic tunability of single-nanocrystal spectral linewidths.

Nat. Chem. 5, 602-606 (2013)

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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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