Volume 222, 2020

Power-dependent photoluminescence decay kinetics of silicon nanocrystals under continuous and pulsed excitation

Abstract

Power-dependent photoluminescence (PL) decay kinetics of silicon nanocrystals (Si NCs) in solid and liquid samples were studied under cw and pulsed excitation. The lifetime distribution and, consequently the measured PL kinetics are shown to depend on the excitation pulse duration until it is not sufficiently short (pulsed limit) or long (cw limit). These two excitation limits, however, are proven to excite different distributions of lifetime components and cannot be directly compared. We derive and experimentally confirm the equality of lifetimes averaged over amplitude and intensity for cw and pulsed excitation, accordingly. The absorption cross section (ACS) of Si NCs in solid and liquid samples is assessed and compared by two approaches under cw-excitation based on the treatment of power-modulated PL kinetics or PL amplitude saturation curves under low and moderate excitation powers, respectively. The discrepancy in extracted ACS values as well as the long-debated phenomena of incomplete PL saturation of matrix-embedded Si NCs is explained by a proposed model that is based on saturation of various components in an ensemble distribution at different excitation powers. The model finally allows us to explain the mystery of average decay lifetime dependence on excitation power in the non-linear power regime. By varying the excitation from cw to pulsed, we showed the reduction of average decay lifetime in the later case and attribute this to the increased relative PL contribution of fast lifetime components that results in at least one order of magnitude lower ACS values. Finally, exciting the solid sample with very high excitation powers, we detected a PL intensity decrease region that allowed us to extract the Auger lifetime which is about 170 ns.

Graphical abstract: Power-dependent photoluminescence decay kinetics of silicon nanocrystals under continuous and pulsed excitation

Associated articles

Article information

Article type
Paper
Submitted
01 Oct 2019
Accepted
01 Nov 2019
First published
01 Nov 2019

Faraday Discuss., 2020,222, 274-293

Power-dependent photoluminescence decay kinetics of silicon nanocrystals under continuous and pulsed excitation

M. Greben and J. Valenta, Faraday Discuss., 2020, 222, 274 DOI: 10.1039/C9FD00100J

To request permission to reproduce material from this article, please go to the Copyright Clearance Center request page.

If you are an author contributing to an RSC publication, you do not need to request permission provided correct acknowledgement is given.

If you are the author of this article, you do not need to request permission to reproduce figures and diagrams provided correct acknowledgement is given. If you want to reproduce the whole article in a third-party publication (excluding your thesis/dissertation for which permission is not required) please go to the Copyright Clearance Center request page.

Read more about how to correctly acknowledge RSC content.

Social activity

Spotlight

Advertisements