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Figure 1.

Synthesis of trimeric imidazoquinoline dendrimer 3.

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Figure 2.

Synthesis of Click reaction derived imidazoquinoline dendrimer 8.

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Figure 3.

TLR7- and TLR8-agonism and IFN-α and IFN-γ induction by Compounds 3, 4, and 8.

Top: TLR7- and TLR8-agonistic activity. Reporter gene assays specific for human TLR7 and TLR8 were used. Data points represent means and SD of quadruplicates. Bottom: IFN-α and IFN-γ induction by Compounds 4 and 8 in human PBMCs, assayed by analyte-specific ELISAs. Data points represent means of duplicates of three representative experiments.

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Figure 4.

Cytokine induction by Compounds 4 and 8 in human PBMCs.

Data points of dose-response profiles represent means of duplicates of three representative experiments. Cytokines were quantified using cytometric bead array assays.

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Figure 5.

Anti-bovine α-lactalbumin-specific IgG titers.

Top: Anti-bovine α-lactalbumin-specific IgG titers in rabbits adjuvanted with 4, 8, a TLR7-specific imidazoquinoline (1-benzyl-2-butyl-1H-imidazo[4,5-c]quinolin-4-amine; reported as Compound 31 in Ref. 9), and unadjuvanted controls (n = 3 per cohort). Ratios of immune/pre-immune titers yielding absorbance values of 1.0 are shown for the individual samples. Each symbol corresponds to the titer of a single animal. Bottom: Chaotropic ELISA showing apparent titers as a function of chaotrope (NaSCN) concentration. Means and SD are shown.

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Figure 6.

Linear peptide epitope mapping results of immune sera.

Top: Foreground fluoresence intensities of secondary goat anti-rabbit IgG (H+L) conjugated with DyLight680 antibody to each overlapping 13-mer peptide in the microarray are shown (means and SD). Bottom: Raw fluorescence images of representative peptide microarrays are shown. Each array is framed by a fusion tag (Flag) peptide (DYKDDDDKGG, 72 red spots) and influenza virus hemagglutinin (HA) epitope tag peptide (YPYDVPDYAG, 72 green spots) which were used as internal controls.

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Figure 7.

Mapping of immunoreactive linear epitopes of bovine α-lactalbumin to its primary sequence and crystal structure.

Top: Sequence homology between bovine and rabbit α-lactalbumin. Conservative and non-conservative changes are shown in blue and red, respectively. Bottom: Mapping of immunoreactive linear epitopes to the crystal structure of bovine α-lactalbumin (PDB code: 1F6R). Regions colored green show contiguous immunodominant epitopes elicited by both 4 and 8, while regions colored red show additional epitopes specifically adjuvanted by 8.

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Figure 8.

Correlation of observed and predicted epitopes.

Overlay of normalized mean background-corrected fluorescence intensity (13-mer peptide-specific immunoreactivity) of the dendrimer 8-adjuvanted rabbit sera and normalized Parker Hydrophilicity parameter computed with a moving window of 13 residues.

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