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The newly developed van der Waals materials allow fabrication of multilayer heterostructures. Early efforts have mostly focused on heterostructures formed by similar materials. More recently, however, attempts have been made to expand the types of materials, such as topological insulators and organic semiconductors. Here we introduce an amorphous semiconductor to the material library for constructing van der Waals heterostructures. Samples composed of 2 nm amorphous black phosphorus synthesized by pulsed laser deposition and monolayer WS 2 obtained by mechanical exfoliation were fabricated by dry transfer. Photoluminescence measurements revealed that photocarriers excited in WS 2 of the heterostructure transfer to amorphous black phosphorus, in the form of either energy or charge transfer, on a time scale shorter than the exciton lifetime in WS 2 . Transient absorption measurements further indicate that holes can efficiently transfer from WS 2 to amorphous black phosphorus. However, interlayer electron transfer in either direction was found to be absent. The lack of electron transfer from amorphous black phosphorus to WS 2 is attributed to the localized electronic states in the amorphous semiconductor. Furthermore, we show that a hexagonal BN bilayer can effectively change the hole transfer process. 

We report a combined theoretical and experimental study on photocarrier dynamics in monolayer phosphorene and bulk black phosphorus. Samples of monolayer phosphorene and bulk black phosphorus were fabricated by mechanical exfoliation, identified according to their reflective contrasts, and protected by covering them with hexagonal boron nitride layers. Photocarrier dynamics in these samples was studied by an ultrafast pump–probe technique. The photocarrier lifetime of monolayer phosphorene was found to be about 700 ps, which is about 9 times longer than that of bulk black phosphorus. This trend was reproduced in our calculations based on ab initio nonadiabatic molecular dynamics combined with time-domain density functional theory in the Kohn–Sham representation, and can be attributed to the smaller bandgap and stronger nonadiabatic coupling in bulk. The transient absorption response was also found to be dependent on the sample orientation with respect to the pump polarization, which is consistent with the previously reported anisotropic absorption of phosphorene. In addition, an oscillating component of the differential reflection signal at early probe delays was observed in the bulk sample and was attributed to the layer-breathing phonon mode with an energy of about 1 meV and a decay time of about 1.35 ps. These results provide valuable information for application of monolayer phosphorene in optoelectronics.