Monolayer transition-metal dichalcogenide crystals (TMDC) can be combined with other functional materials, such as organic molecules, to from a wide range of heterostructures with tailorable properties. Although a number of works have shown that ultrafast charge transfer (CT) can occur at organic-TMDC interfaces, conditions that would facilitate the separation of interfacial CT excitons into free carriers remain unclear. Here, time-resolved and steady-state photoemission spectroscopy are used to study the potential energy landscape, charge transfer and exciton dynamics at the zinc phthalocyanine (ZnPc)/monolayer (ML) MoS 2 and ZnPc/bulk MoS 2 interfaces. Surprisingly, although both interfaces have a type-II band alignment and exhibit sub-100 femtosecond CT, the CT excitons formed at the two interfaces show drastically different evolution dynamics. The ZnPc/ML-MoS 2 behaves like typical donor-acceptor interfaces in which CT excitons dissociate into electron-hole pairs. On the contrary, back electron transfer occur at ZnPc/bulk-MoS 2 , which results in the formation of triplet excitons in ZnPc. The difference can be explained by the different amount of band bending found in the ZnPc film deposited on ML-MoS 2 and bulk-MoS 2. Our work illustrates that the potential energy landscape near the interface plays an important role in the charge separation behavior. Therefore, considering the energy level alignment at the interface alone is not enough for predicting whether free charges can be generated effectively from an interface.
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.
We report observations of a strong thickness dependence for charge transfer (CT) from MoSe 2 to MoS 2 , as evidenced by transient absorption measurements. By time-resolving CT from MoSe 2 monolayers (1Ls) to MoS 2 flakes of varying thicknesses, including 1L, bilayer (2L), and trilayer (3L), we find that the CT time is several picoseconds in the 1L-MoSe 2 /3L-MoS 2 heterostructure, which is much longer than that of 1L-MoSe 2 /1L-MoS 2 and 1L-MoSe 2 /2L-MoS 2 heterostructures. In addition, the recombination lifetime of the interlayer excitons in the 1L/3L heterostructure is several times longer than that of 1L/1L and 1L/ 2L heterostructures, reaching 800 ps. Furthermore, we show that a prepulse can reduce the CT time and enhance the interlayer exciton recombination in the 1L/3L heterostructure. These findings illustrate that layer thickness can be an important parameter to control the CT property of van der Waals heterostructures. These experimental results also provide important information for further refining the understanding of the physical mechanisms of CT in van der Waals heterostructures.
We report the properties of hybrid deposited iron pyrite (FeS 2) thin films applied as the back contact interface layers of CdS/CdTe solar cells. The hybrid deposition process for FeS 2 optimized in this study relies on DC magnetron sputtering of iron with simultaneous thermal evaporation of sulfur. We have fabricated solar cells incorporating CdS/CdTe window/absorber layers sputter-deposited onto commercial transparent conducting oxide coated glass and have compared the performance of devices incorporating the new FeS 2 /Cu/Au back contacts with that of standard devices incorporating Cu/Au back contacts. Considering our best devices of each type, the inclusion of the FeS 2 thin film as a hole transport layer has improved the open circuit voltage V OC by 2.1%, reaching 817 mV, and the fill-factor FF by 8.3% relative, reaching 74.7%, in comparison with devices omitting the FeS 2 layer. Under standard test conditions of 100 mA/cm 2 simulated AM1.5G and 25 C, devices utilizing the FeS 2 hole transport layer have shown a conversion efficiency as high as 13.3%-a relative increase in of ~10% over our current laboratory standard back contact. The attained FF exceeds previous results for high efficiency sputter-deposited CdS/CdTe solar cells.
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