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Van der Waals heterostructures obtained by artificially stackingtwo-dimensional crystals represent the frontier of material engineering,demonstrating properties superior to those of the starting materials. Finecontrol of the interlayer twist angle has opened new possibilities fortailoring the optoelectronic properties of these heterostructures. Twistedbilayer graphene with a strong interlayer coupling is a prototype of twistedheterostructure inheriting the intriguing electronic properties of graphene.Understanding the effects of the twist angle on its out-of-equilibrium opticalproperties is crucial for devising optoelectronic applications. With this aim,we here combine excitation-resolved hot photoluminescence with femtosecondtransient absorption microscopy. The hot charge carrier distribution induced byphoto-excitation results in peaked absorption bleaching and photo-inducedabsorption bands, both with pronounced twist angle dependence. Theoreticalsimulations of the electronic band structure and of the joint density of statesenable to assign these bands to the blocking of interband transitions at thevan Hove singularities and to photo-activated intersubband transitions. Thetens of picoseconds relaxation dynamics of the observed bands is attributed tothe angle-dependence of electron and phonon heat capacities of twisted bilayergraphene.

Angle-tunable intersubband photoabsorption and enhanced photobleaching in twisted bilayer graphene