Spectral widths and Stokes shifts in InP-based quantum dots

Cavanaugh, Paul; Wang, Xudong; Bautista, Maria J.; Jen-La Plante, Ilan; Kelley, David F.

doi:10.1063/5.0165956

Title: Spectral widths and Stokes shifts in InP-based quantum dots

Journal Article · Tue Oct 03 00:00:00 EDT 2023 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/5.0165956· OSTI ID:2007413

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University of California Merced, CA (United States)
Nanosys, Inc., Milpitas, CA (United States)

InP-based quantum dots (QDs) have Stokes shifts and photoluminescence (PL) line widths that are larger than in II–VI semiconductor QDs with comparable exciton energies. The mechanisms responsible for these spectral characteristics are investigated in this paper. Upon comparing different semiconductors, we find the Stokes shift decreases in the following order: InP > CdTe > CdSe. We also find that the Stokes shift decreases with core size and decreases upon deposition of a ZnSe shell. We suggest that the Stokes shift is largely due to different absorption and luminescent states in the angular momentum fine structure. The energy difference between the fine structure levels, and hence the Stokes shifts, are controlled by the electron–hole exchange interaction. Luminescence polarization results are reported and are consistent with this assignment. Spectral widths are controlled by the extent of homogeneous and inhomogeneous broadening. Here, we report PL and PL excitation (PLE) spectra that facilitate assessing the roles of homogeneous and different inhomogeneous broadening mechanisms in the spectra of zinc-treated InP and InP/ZnSe/ZnS particles. There are two distinct types of inhomogeneous broadening: size inhomogeneity and core–shell interface inhomogeneity. The latter results in a distribution of core–shell band offsets and is caused by interfacial dipoles associated with In–Se or P–Zn bonding. Quantitative modeling of the spectra shows that the offset inhomogeneity is comparable to but somewhat smaller than the size inhomogeneity. The combination of these two types of inhomogeneity also explains several aspects of reversible hole trapping dynamics involving localized In³⁺/V_Zn^2– impurity states in the ZnSe shells.

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Research Organization:: Nanosys, Inc., Milpitas, CA (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0009164

OSTI ID:: 2007413

Journal Information:: Journal of Chemical Physics, Vol. 159, Issue 13; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
InP
quantum dot
emission linewidth
Stokes shift
excitons
phonons
electronic band structure
semiconductors
photoluminescence excitation
photoluminescence spectroscopy

Title: Spectral widths and Stokes shifts in InP-based quantum dots

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