Origin of stretched-exponential photoluminescence relaxation in size-separated silicon nanocrystals

A detailed understanding of the photoluminescence (PL) from silicon nanocrystals (SiNCs) is convoluted by the complexity of the decay mechanism, including a stretched-exponential relaxation and the presence of both nanosecond and microsecond time scales. In this publication, we analyze the microsecond PL decay of size-resolved SiNC fractions in both full-spectrum (FS) and spectrally resolved (SR) configurations, where the stretching exponent and lifetime are used to deduce a probability distribution function (PDF) of decay rates. For the PL decay measured at peak emission, we find a systematic shift and narrowing of the PDF in comparison to the FS measurements. In a similar fashion, we resolve the PL lifetime of the ‘blue’, ‘peak’, and ‘red’ regions of the spectrum and map PL decays of different photon energy onto their corresponding location in the PDF. A general trend is observed where higher and lower photon energies are correlated with shorter and longer lifetimes, respectively, which we relate to the...