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Hybrid quantum dot (QD) / transition metal dichalcogenide (TMD)heterostructures are attractive components of next generation optoelectronicdevices, which take advantage of the spectral tunability of QDs and the chargeand exciton transport properties of TMDs. Here, we demonstrate tunableelectronic coupling between CdSe QDs and monolayer WS$_2$ using variable lengthalkanethiol ligands on the QD surface. Using femtosecond time-resolved secondharmonic generation (SHG) microscopy, we show that electron transfer fromphotoexcited CdSe QDs to single-layer WS$_2$ occurs on ultrafast (50 fs - 1 ps)timescales. Moreover, in the samples exhibiting the fastest charge transferrates ($\leq$ 50 fs) we observed oscillations in the time-domain signalcorresponding to an acoustic phonon mode of the donor QD, which coherentlymodulates the SHG response of the underlying WS$_2$ layer. These results revealsurprisingly strong electronic coupling at the QD/TMD interface and demonstratethe usefulness of time-resolved SHG for exploring ultrafastelectronic-vibrational dynamics in TMD heterostructures.

Ultrafast Charge Transfer at a Quantum Dot/2D Materials Interface Probed by Second Harmonic Generation