EPR and structural characterization of water-soluble mn2+-doped si nanoparticles

Tonya M. Atkins, Jeffrey H. Walton, Mani P. Singh, Shreyashi Ganguly, Oliver Janka, Angelique Y. Louie, Susan M. Kauzlarich

Research output: Contribution to journalArticle

4 Scopus citations

Abstract

Water-soluble poly(allylamine) Mn2+-doped Si (SiMn) nanoparticles (NPs) were prepared and show promise for biologically related applications. The nanoparticles show both strong photoluminescence and good magnetic resonance contrast imaging. The morphology and average diameter were obtained through transmission electron microscopy (TEM) and high-resolution transmission electron microscopy (HRTEM); spherical crystalline Si NPs with an average diameter of 4.2 ± 0.7 nm were observed. The doping maximum obtained through this process was an average concentration of 0.4 ± 0.3% Mn per mole of Si. The water-soluble SiMn NPs showed a strong photoluminescence with a quantum yield up to 13%. The SiMn NPs had significant T1 contrast with an r1 relaxivity of 11.1 ± 1.5 mM-1 s-1 and r2 relaxivity of 32.7 ± 4.7 mM-1 s-1 where the concentration is in mM of Mn2+. Dextran-coated poly(allylamine) SiMn NPs produced NPs with T1 and T2 contrast with a r1 relaxivity of 27.1 ± 2.8 mM-1 s-1 and r2 relaxivity of 1078.5 ± 1.9 mM-1 s-1. X-band electron paramagnetic resonance spectra are fit with a two-site model demonstrating that there are two types of Mn2+ in these NP’s. The fits yield hyperfine splittings (A) of 265 and 238 MHz with significant zero field splitting (D and E terms). This is consistent with Mn in sites of symmetry lower than tetrahedral due to the small size of the NP’s.

Original languageEnglish (US)
Pages (from-to)1948-1956
Number of pages9
JournalJournal of Physical Chemistry C
Volume121
Issue number3
DOIs
StatePublished - 2017
Externally publishedYes

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry

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    Atkins, T. M., Walton, J. H., Singh, M. P., Ganguly, S., Janka, O., Louie, A. Y., & Kauzlarich, S. M. (2017). EPR and structural characterization of water-soluble mn2+-doped si nanoparticles. Journal of Physical Chemistry C, 121(3), 1948-1956. https://doi.org/10.1021/acs.jpcc.6b11000