Maybe you found the answer a long time ago but given the fact that I found very little on this topic when searching for a way to colorize the bars of a chart I thought it might be useful to post the solution here when it opened up to me.
It seems that the implementation of System.Web.Helpers.Chart is closely related to System.Web.UI.DataVisualization.Charting.Chart. Given this, I managed to find some clues as to how I could configure the "theme" XML properties:
public const String CHARTS_THEME = @"<Chart BackColor=""#EFEFEF"" BackGradientStyle=""TopBottom"" BorderColor=""#A0A0A0"" BorderWidth=""1"" Palette=""None"" PaletteCustomColors=""#ffcc00"" >
<ChartAreas>
<ChartArea Name=""Default"" _Template_=""All"" BackColor=""Transparent"" BackSecondaryColor=""White"" BorderWidth=""1"" BorderColor=""#A0A0A0"" BorderDashStyle=""Solid"" >
<AxisY>
<MajorGrid Interval=""Auto"" LineColor=""64, 64, 64, 64"" />
<LabelStyle Font=""Verdana, 10pt"" />
</AxisY>
<AxisX LineColor=""#000000"">
<MajorGrid Interval=""Auto"" LineColor=""64, 64, 64, 64"" />
<LabelStyle Font=""Verdana, 10pt"" />
</AxisX>
</ChartArea>
</ChartAreas>
<Legends>
<Legend _Template_=""All"" BackColor=""Transparent"" Docking=""Bottom"" Font=""Verdana, 10pt, style=Plain"" LegendStyle=""Row"">
</Legend>
</Legends>
</Chart>";
Key to this point is to define your own PaletteCustomColors (I have only one color). To make this work, the Palette property must be set to None.
Finally, just use your theme when creating an instance of your chart:
Chart chart = new Chart(width: 600, height: 200, theme:CHARTS_THEME);
Also check out the msdn documentation of System.Web.UI.DataVisualization.Charting.Chart to discover other ways to style your chart:
http://msdn.microsoft.com/en-us/library/dd467201.aspx