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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. 

Starting with the discovery of graphene in 2004, the interest in two‐dimensional materials since then has been exponentially growing. Across many disciplines, their exceptional electrical, chemical, thermal, and optical properties have drawn considerable attention that has created an entire field within a decade of their discovery. Driven by the mechanical exfoliation technique that allows for the quick exploration of these two‐dimensional materials and their novel devices, joint efforts have been made in order to understand and exploit their potential, consequently leading to the development of their large‐scale growth. This review focuses on recent studies using ultrafast laser spectroscopy that have revealed the photocarrier dynamics in two‐dimensional materials and laid the foundation of their behavior. We provide a brief introduction on ultrafast laser spectroscopy, discuss several aspects of the photocarrier dynamics, and conclude with our perspective on future developments.