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Optics Express

Disentangling the effects of clustering and multi-exciton emission in second-order photon correlation experiments

Benjamin D. Mangum, Yagnaseni Ghosh, Jennifer Ann Hollingsworth, Han Htoon

Published Mar 18, 2013• 85 citations

Abstract

In single particle spectroscopy, the degree of observed fluorescence anti-bunching in a second-order cross correlation experiment is indicative of its bi-exciton quantum yield and whether or not a particle is well isolated. Advances in quantum dot synthesis have produced single particles with bi-exciton quantum yields approaching unity. Consequently, this creates uncertainty as to whether a particle has a high bi-exciton quantum yield or if it exists as a cluster. We report on a time-gated anti-bunching technique capable of determining the relative contributions of both multi-exciton emission and clustering effects. In this way, we can now unambiguously determine if a particle is single. Additionally, this time-gated anti-bunching approach provides an accurate way for the determination of bi-exciton lifetime with minimal contribution from higher order multi-exciton states.

DOI: 10.1364/oe.21.007419

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Recognition of single quantum dots (QDs) from high multi-exciton emission and clustering effects is challenging using the conventional second-order correlation function method. Here we demonstrate a method for fast recognizing single QDs based on the probabilities of detecting single- and two-photon events. The time-tagged, time-resolved and time-correlated single-photon counting technique is applied to effectively remove multi-exciton emission and low-counting background. By this way, single QDs can be fastly recognized by the spatial coincidence-counting model. In addition, the fast recognition of single QDs by using the collected photons during the confocal scanning imaging process has been achieved synchronously.

We report photon correlation measurements that reveal unique signatures of biexciton and charged exciton emissions in a single self-assembled InAs quantum dot. Biexciton emission exhibits both bunching and antibunching under continuous-wave excitation and only antibunching under pulsed excitation. Cross correlation between biexciton and single-exciton emissions reveals highly asymmetric features due to cascaded emission. Under our excitation conditions, no polarization correlations between the exciton and biexciton emissions were observed.

We report the observed photon bunching statistics of biexciton cascade emission at zero time delay in single quantum dots by second-order correlation function g (2) (τ) measurements under continuous wave excitation. It is found that the bunching phenomenon is independent of the biexciton binding energy when it varies from 0.59 meV to nearly zero. The photon bunching takes place when the exciton photon is not spectrally distinguishable from the biexciton photon, and either of them can trigger the 'start' in a Hanbury–Brown and Twiss setup. However, if the exciton energy is spectrally distinguishable from the biexciton, the photon statistics will become asymmetric and a cross-bunching lineshape can be obtained. The theoretical calculations based on a model of three-level rate-equation analysis are consistent with the result of g (2) (τ) correlation function measurements.

The fluorescence of single colloidal CdSe quantum dots is investigated at room temperature by means of the autocorrelation function over a time scale of almost 12 orders of magnitude. At short time, the autocorrelation function shows a complete antibunching indicating single photon emission and atomic-like behavior. On longer time scales (up to tens of seconds), we measure a bunching effect due to fluorescence intermittency that can not be described by fluctuations between two states with constant rates. The autocorrelation function also exhibits a non-stationary behavior related to power-law distributions of "On" and "Off" times.

The fluorescence of single-colloidal CdSe quantum dots is investigated at room temperature by means of the autocorrelation function over a time scale of almost 12 orders of magnitude. Over a short time scale, the autocorrelation function shows complete antibunching, indicating single-photon emission and atomiclike behavior. Over longer time scales (up to tens of seconds), we measure a bunching effect that is due to fluorescence intermittency and that cannot be described by fluctuations between two states with constant rates. The autocorrelation function also exhibits nonstationary behavior related to power-law distributions of On and Off times.