Preheat the oven to 300 degrees F. Lightly coat six 6-ounce ramekins with cooking spray.
Prepare the custard, by adding the milk, cream, and espresso powder into a 1 1/2-quart, nonreactive heavy-bottomed saucepan and warm over medium-high heat. While the cream mixture is heating, use a sharp paring knife to slice the vanilla bean pod in half lengthwise. Separate the beans from the pod by scraping the inside of the pod with the edge of the knife. Add the beans and pod to the heating cream mixture. (Or substitute and use vanilla bean paste or vanilla extract.) Bring to a boil and immediately remove the saucepan from the heat.
In a large mixing bowl, whisk the egg yolks and the 2/3 cup sugar until well combined. Continue to whisk while slowly pouring the hot cream into the egg mixture. Blend thoroughly. Pour the custard through a fine-mesh sieve to remove the vanilla bean pod and any bits of overcooked egg.
Chocolate-covered espresso beans, for garnish
Place the prepared ramekins in a baking pan with sides that are at least 2 inches high. Pour the custard into the ramekins, filling each halfway. Transfer the baking pan carefully to the oven and fill the ramekins as close to the top as possible without spilling. Fill a measuring cup with hot tap water.
Add enough water to the baking pan to reach three-quarters of the way up the sides of the ramekins.
Bake the custards about 1 hour. Check periodically to make sure the custards are not browning or bubbling. If they are, decrease the temperature to 250 degrees. The custards are done when just set (they should tremble slightly when shaken). If they still looks liquidy, return to the oven for 5 minutes longer, or until set.
Remove the ramekins from the baking pan and cool for 30 to 40 minutes. Cover tightly and refrigerate at least 3 to 4 hours. The custards will firm up in the fridge.
Just before serving, use about 1/2 cup sugar to top each custard with a thin layer of sugar. It is important to spread the sugar evenly and to make sure the sugar layer is thick enough. If you have a kitchen torch, use it to caramelize the sugar. If not, preheat the broiler. Place the ramekins 4 inches from the flame and broil, watching carefully, until the sugar is caramelized and lightly browned. Garnish with chocolate-covered espresso beans and serve immediately.
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