Characterization of PFCE-PLGA-NPs and core-shell PFCE-PLGA-capsules loaded with different gadolinium chelates. (a, b) Gadolinium-content versus mass m of gadolinium used for preparation of nanoparticles determined by ICP-MS: (a) fractal multicore nanoparticles, (b) core-shell nanocapsules. When lipophilic gadolinium chelates are used, gadolinium content in nanoparticles increases with increased amount of gadolinium chelate added during the emulsification. In contrast, the encapsulation of Prohance was lower with 0.10 µg!mg(NP) -1 in multicore nanoparticles and 0.11 µg!mg(NP) -1 in capsules despite that 140 mg Gd were used for encapsulation (not shown for clarity). (c, d) PFCE-content determined by 19 F NMR spectroscopy (trifluoroacetic acid as an internal reference, D2O, 378 MHz). In multicore nanoparticles (c), the encapsulation of PFCE seem to decrease with an increasing loading of gadolinium chelates. In contrast, the PFCE content in nanocapsules (d) remains constant with an increasing Gd-content. See Table S3 and S4.

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... fractal multicore nanoparticles and core-shell nanocapsules can be produced in a miniemulsion formulation approach, 26 Table S1). The capsules were slightly smaller and had diameters of 150-180 nm (Table S2) When lipophilic chelates were used for the synthesis, the concentration of encapsulated gadolinium increased in both fractal multicore and core-shell particles with the added amount chelate, as shown by inductively coupled plasma-mass spectrometry (ICP-MS, Figure 2a, b). The encapsulation of Gd_02 that has a longer hydrophobic chain was slightly higher compared to Gd_01. ...

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... S3 and S4. The encapsulation of PFCE showed different trends in fractal multicore nanoparticles and coreshell nanocapsules, as shown by a quantitative 19 F NMR spectroscopy (Figure 2c, d). Thus, the PFCE-content in multicore nanoparticles appears to decrease with increasing concentration of Gd(III) (Figure 2c). ...

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... encapsulation of PFCE showed different trends in fractal multicore nanoparticles and coreshell nanocapsules, as shown by a quantitative 19 F NMR spectroscopy (Figure 2c, d). Thus, the PFCE-content in multicore nanoparticles appears to decrease with increasing concentration of Gd(III) (Figure 2c). This trend was not observed in nanocapsules. ...

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... the content was even higher compared to capsules that did not contain gadolinium chelate. (Figure 2c, d). However, it is important to note that the encapsulation of paramagnetic chelates can have different effects on the MR properties in both types of particles. ...

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... stark increase of the transverse relaxation rate in multicore nanoparticles can cause the differences in the quantification of PFCE between fractal multicore nanoparticles and core-shell nanocapsules (compare Figure 2c and d). A shorter transverse relaxation time T2 always leads to line broadening of the NMR signal (see Figures S4 and S5). ...