11.07.2015 Views

Copyright 2004 by Marcel Dekker, Inc. All Rights Reserved.

Copyright 2004 by Marcel Dekker, Inc. All Rights Reserved.

Copyright 2004 by Marcel Dekker, Inc. All Rights Reserved.

SHOW MORE
SHOW LESS

You also want an ePaper? Increase the reach of your titles

YUMPU automatically turns print PDFs into web optimized ePapers that Google loves.

high-threshold e–h plasma mechanisms. Thermal dissociation of excitons atroom temperature (the exciton binding energy in CdSe is 16 meV) results in asignificantly increased threshold for light amplification. Because of a largeinterlevel spacing, ‘‘quantum-confined’’ excitons in NQDs are more robustthan bulk excitons, allowing one to excite room-temperature ASE at pumplevels comparable to those at cryogenic temperatures. This is an illustrativeexample of the enhanced temperature stability of optical gain expected forstrongly confined NQDs.B. Modal Gain StudiesOne of the most direct ways of quantifying optical-gain properties ofmaterials is <strong>by</strong> using ‘‘variable-stripe-length’’ measurements of ASE [61]. Inthese measurements, the excitation beam is focused onto the sample with acylindrical lens into a narrow stripe of variable length l and the emissionintensity is monitored as a function of the stripe length (see inset in Fig. 25a).This experiment allows one to determine net or modal gain ( g m ), whichrepresents a difference between material gain ( g) and linear optical losses due,for example, to light scattering.Figure 25a shows a set of room-temperature emission spectra for a CdSeNQD film (mean dot radius R = 2.5 nm) recorded using a ‘‘variable-stripelength’’configuration. The development of ASE (a narrow peak at f635 nm)occurs at a threshold stripe length, l th , of f0.06 cm. The ASE threshold isclearly seen in the plot of the emission intensity (I) versus the stripe length as asharp increase in the slope at l>l th (Fig. 25b). To derive the magnitude ofmodal gain, the I-versus-l dependence is usually analyzed using the expressionI = A(e g ml 1)/g m , in which A is a constant proportional to the spontaneousemission power density [61]. This dependence should, in principle, describeboth an initial, linear intensity growth below the ASE threshold (spontaneousemission regime) and a fast, exponential increase above it (stimulatedemission regime). However, in the case of NQD samples, this simple expressiondoes not allow one to simultaneously fit both regimes (see fit shown <strong>by</strong>dashed line in Fig. 25b). This discrepancy is fundamentally linked to the factthat in NQDs, spontaneous and stimulated emission arise from different typesof excitation.As indicated <strong>by</strong> the analysis in previous sections, optical gain and hence,stimulated emission in NQDs are dominated <strong>by</strong> quantum-confined biexcitons(doubly-excited dots). However, because of their short lifetimes, which arelimited <strong>by</strong> nonradiative Auger recombination, biexcitons are not pronouncedin spontaneous emission. Simple estimations based on the comparison ofefficiencies of Auger decay and radiative recombination indicate that thecontribution of biexcitons to time-integrated spontaneous emission is less<strong>Copyright</strong> <strong>2004</strong> <strong>by</strong> <strong>Marcel</strong> <strong>Dekker</strong>, <strong>Inc</strong>. <strong>All</strong> <strong>Rights</strong> <strong>Reserved</strong>.

Hooray! Your file is uploaded and ready to be published.

Saved successfully!

Ooh no, something went wrong!