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Title: Optical phonons in nanostructured thin films composed by zincblende zinc selenide quantum dots in strong size-quantization regime: Competition between phonon confinement and strain-related effects

Raman scattering in combination with optical spectroscopy and structural studies by X-ray diffraction was employed to investigate the phonon confinement and strain-induced effects in 3D assemblies of variable-size zincblende ZnSe quantum dots close packed in thin film form. Nanostructured thin films were synthesized by colloidal chemical approach, while tuning of the nanocrystal size was enabled by post-deposition thermal annealing treatment. In-depth insights into the factors governing the observed trends of the position and half-width of the 1LO band as a function of the average QD size were gained. The overall shifts in the position of 1LO band were found to result from an intricate compromise between the influence of phonon confinement and lattice strain-induced effects. Both contributions were quantitatively and exactly modeled. Accurate assignments of the bands due to surface optical (SO) modes as well as of the theoretically forbidden transverse optical (TO) modes were provided, on the basis of reliable physical models (such as the dielectric continuum model of Ruppin and Englman). The size-dependence of the ratio of intensities of the TO and LO modes was studied and discussed as well. Relaxation time characterizing the phonon decay processes in as-deposited samples was found to be approximately 0.38 ps, whilemore » upon post-deposition annealing already at 200 °C it increases to about 0.50 ps. Both of these values are, however, significantly smaller than those characteristic for a macrocrystalline ZnSe sample. - Graphical abstract: Optical phonons in nanostructured thin films composed by zincblende zinc selenide quantum dots in strong size-quantization regime: competition between phonon confinement and strain-related effects. - Highlights: • Phonon confinement vs. strain-induced effects in ZnSe 3D QD assemblies were studied. • Shifts of the 1LO band result from an intricate compromise between the two effects. • SO and theoretically forbidden TO modes were accurately assigned. • Phonon relaxation time in as-deposited and annealed samples is 0.38 ps and 0.50 ps. • Both values are significantly smaller than in macrocrystalline ZnSe sample.« less
Authors:
Publication Date:
OSTI Identifier:
22334196
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Solid State Chemistry; Journal Volume: 213; Other Information: Copyright (c) 2014 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 77 NANOSCIENCE AND NANOTECHNOLOGY; DEPOSITION; DEPOSITS; PHONONS; QUANTUM DOTS; RAMAN EFFECT; RAMAN SPECTRA; SEMICONDUCTOR MATERIALS; SPECTROSCOPY; THIN FILMS; X-RAY DIFFRACTION; ZINC; ZINC SELENIDES; ZINC SULFIDES