Time-resolved studies of fluorescence and band-edge charge carrier dynamics in In1-xGaxP colloidal quantum dots

Alexander A. Mikhailovsky; Frederic S. Diana; Sangcheol Kim; Edward J. Kramer; Pierre M. Petroff; Jeffrey Gerbec; Geoffrey Strouse

doi:10.1117/12.616419

18 August 2005 Time-resolved studies of fluorescence and band-edge charge carrier dynamics in In_1-xGa_xP colloidal quantum dots

Alexander A. Mikhailovsky, Frederic S. Diana, Sangcheol Kim, Edward J. Kramer, Pierre M. Petroff, Jeffrey Gerbec, Geoffrey Strouse

Author Affiliations +

Proceedings Volume 5929, Physical Chemistry of Interfaces and Nanomaterials IV; 59290R (2005) https://doi.org/10.1117/12.616419
Event: Optics and Photonics 2005, 2005, San Diego, California, United States

Abstract

In this submission, we report on the results of spectroscopic studies of charge carrier dynamics in colloidal In_1-xGa_xP quantum dots (QDs) with low levels of Ga doping (x~1%). These QDs exhibit large global Stokes shift of fluorescence (up to 300 meV) along with high emission yield (up to 30% in solution and 25% in films under blue excitation at 300 K) after post-synthesis photo-chemical treatment. In order to reveal the nature of large fluorescence Stokes shift and study the band-edge carriers dynamics, we performed time-resolved measurements of emission and photo-induced absorption changes in QDs with different sizes and surface passivation. The work was focused on the studies of differences between QDs subjected to photochemical surface passivation and bare nanoparticles. Time-resolved absorption spectroscopy indicates that holes' trapping strongly depends on passivation of surface trap states and can even suppress Auger multiparticle recombination in poorly passivated nanoparticles. Transient fluorescence measurements in well-passivated nanoparticles demonstrate that at short delays (<2 ns), emission Stokes shift is almost twice smaller than in steady-state measurements and matches the emission band in unpassivated QDs. At longer delays, time-resolved emission matches the spectra obtained with continuous wave (CW) excitation. We propose that initially photoluminescence occurs from quantum-confined state and subsequent hole relaxation onto surface/interface sites gives rise to emission with large global Stokes shift. In poorly passivated QDs, holes escape quickly to deep-trap states that leads to formation of low-efficiency broad emission band red-shifted with respect to the excitonic PL band.

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Alexander A. Mikhailovsky, Frederic S. Diana, Sangcheol Kim, Edward J. Kramer, Pierre M. Petroff, Jeffrey Gerbec, and Geoffrey Strouse "Time-resolved studies of fluorescence and band-edge charge carrier dynamics in In_1-xGa_xP colloidal quantum dots", Proc. SPIE 5929, Physical Chemistry of Interfaces and Nanomaterials IV, 59290R (18 August 2005); https://doi.org/10.1117/12.616419

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KEYWORDS

Indium gallium phosphide

Luminescence

Nanoparticles

Absorption

Gallium

Picosecond phenomena

Carrier dynamics

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