This is a hard question to respond to.
Many things might make someone grumpy. There are also individual temperaments, making grumpy hard to quantify - a Grumpy to one person might barely be a blip on another individual's scale. Hormones like cortisol reflect stress, and can make people in general irritable, but I doubt any one combination of hormones would always cause grumpiness.
But I thought I'd venture an answer since I did see this paper today: "Low glucose relates to greater aggression in married couples" doi: 10.1073/pnas.1400619111
Being hungry will do this for lots of people, so maybe a bit of an answer for you. There are lots of different kinds of signals that mediate hunger though, so still a tough call.
Update: here's an additional article that specifically talks about parts of the brain involved in aggression and grumpiness as response to a drop in glucose.