Heat oven to 350°F. Grease and lightly flour 2 (9-inch) round cake pans; set aside.
Combine sugar and 3/4 cup butter in bowl; beat at medium speed, scraping bowl often, until creamy. Add cooled chocolate, eggs and 2 teaspoons vanilla; continue beating until well mixed. Add flour, baking soda, baking powder and salt to butter mixture alternately with 1 1/3 cups coffee, beating at low speed just until well mixed.
Pour batter evenly into prepared pans. Bake 20-30 minutes or until toothpick inserted in center comes out clean. Cool 10 minutes. Remove from pans. Cool completely.
Beat 2/3 cup butter in bowl at medium speed until creamy. Gradually add powdered sugar, cocoa, vanilla and enough coffee for desired spreading consistency; beat well after each addition.
Place 1 cake layer onto serving plate. Spread 1/2 cup frosting over top; top with second cake layer. Spread remaining frosting over top and sides of cake..
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