Heat oven to 325°. In a medium bowl, melt the chocolate and butter together over a pot of barely simmering water or in short bursts in the microwave. Stir to combine, then set aside to cool slightly. Stir in the orange zest, egg yolks, vanilla, and salt. Stir in the cocoa powder.
Using an electric mixer, beat the egg whites to soft peaks in a clean large bowl. Gradually add the sugar and beat until shiny stiff peaks form, about 2 minutes. Stir a scoop of the egg white mixture into the chocolate mixture to loosen it, then carefully fold in the remainder.
Divide the batter between four (4 oz.) ramekins and smooth the tops. Set the ramekins on a baking sheet. Bake until the cakes are puffed and the tops look dry but the centers are still moist, 20 to 22 minutes. Serve warm.
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