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Directions:
Toast walnuts in a 350º F oven for 5 to 10 minutes.
In a food processor coarsely chop 3 cups walnuts for crust. Place chopped walnuts in a bowl, add 2 tablespoons of the simple syrup and the melted butter, mix well. Place mixture in a 10 inch fluted tart pan with removable bottom and press into pan with your fingers to form a crust. Put pan in freezer to firm while you complete the next step (about 10 minutes).
Use a knife to break chocolate into small shards. In a medium saucepan bring cream to a boil, add chocolate and remove from heat. Stir until smooth. Stir in Grand Marnier. Pour mixture into chilled tart mold and refrigerate for 4 hours or overnight.
In a small nonstick saute pan, combine the remaining 2 tablespoons simple syrup and the orange zest. Cook over medium heat until most of the water has evaporated and the zest is translucent, 2 to 3 minutes. Remove from pan and cool.
Keep chilled until ready to serve. Remove tart from pan. To slice, use a knife dipped in hot water and wiped with a towel. Garnish slices with powdered sugar-dusted walnut halves and candied orange zest.
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