Since the LabelDefinitions collection of the series is not available in the Style's Setters' properties you use an attached property to add the label definition in it. You can see the Label Template Customization example that demonstrates such approach. Please give it a try and let me know if it works for you. As a side note, the example is in Silverlight, but it shares its code with the WPF version and the used approach for the label definition is the same.
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I am trying to do something very similar and the proposed solution works fine but now i want to rotate the text of the label to display vertically. I know this is the WPF forum, but I am trying to do this in Silverlight. I have tried the following: