Ultrafast Drift Current Terahertz Emission Amplification in the Monolayer WSe2/Si Heterostructure.

Two-dimensional transition metal dichalcogenides (TMDs) have great potential application for seamless on-chip integration due to their strong photon-electron-spin-valley coupling. However, the contact-free measurements of the valley-coupled photocurrent in TMDs is still challenging. Here, ultrafast terahertz emission spectroscopy is employed to investigate the photocurrent dynamics in monolayer WSe2, and an interface-induced drift current amplification is found in the WSe2/Si heterostructure. The amplification of terahertz emission comes from the photocurrent enlarged by band bending in the WSe2 and Si junction, and the amplification ratio increase further near the valley resonant transition of WSe2. In addition, the valley-momentum locked photocurrent in the WSe2/Si heterostructure reserves the same chirality with monolayer WSe2 at room temperature. These findings could provide a new method for manipulating valley-momentum locked photocurrent by photon helicity and open new avenues for TMD-based valley-polarized terahertz emission devices.

Tunable ultrafast electron transfer in WSe2-graphene heterostructures enabled by atomic stacking order.

Efficient interfacial light-electric interconversion in van der Waals (vdW) heterostructures is crucial for their optoelectronic applications. However, an in-depth understanding of the necessary process for device operation, namely interfacial charge transfer (CT), has thus far remained elusive. In this study, by using photon energy-dependent transient THz spectroscopy, we complementarily investigate the interfacial CT process in heterostructures comprising monolayers of WSe2 and graphene with varying stacking orders on a sapphire substrate. We observe that the CT mechanism of the sub-A-exciton excitation is different from that of the above-A-exciton excitation. Notably, the CT process occurs via a photo-thermionic emission for sub-A-exciton excitations and a direct electron (or hole) transfer for above-A-exciton excitations. Furthermore, we demonstrate that the effective electric field induced by the sapphire substrate could adjust the Schottky barrier from a p-type contact (WSe2/Gr/sapphire) to an n-type contact (Gr/WSe2/sapphire). Consequently, it is more beneficial for the photo-thermionic electrons to transfer from graphene to WSe2 over the Schottky barrier in Gr/WSe2/sapphire. These results can provide new insights into the CT process in graphene-transition metal dichalcogenide (TMDC) vdW interfaces, which are critical to potential optoelectronic applications of graphene-TMDC heterostructures.

Hot Carrier Transfer in PtSe2/Graphene Enabled by the Hot Phonon Bottleneck.

The charge transfer (CT) process of two-dimensional (2D) graphene/transition metal dichalcogenides (TMDs) heterostructures makes the photoelectric conversion ability of TMDs into a wider spectral range for the light harvester and photoelectric detector applications. However, the direct in situ investigation of the hot carrier transport in graphene/TMDs heterostructures has been rarely reported. Herein, using the optical pump and a terahertz (THz) probe (OPTP) spectroscopy, the CT process from graphene to five-layer PtSe2 in the PtSe2/graphene (P/G) heterostructure is demonstrated to be related to the pump fluence, which is enabled by the hot phonon bottleneck (HPB) effect in graphene. Furthermore, the frequency dispersion conductivity and the THz emission spectroscopy of the P/G heterostructure confirmed the existence of interlayer CT and its pump fluence-dependent behavior. Our results provide in-depth physical insights into the CT mechanism at the P/G van der Waals interface, which is crucial for further exploration of optoelectronic devices based on P/G heterostructures.

Ultrafast Charge Generation Enhancement in Nanoscale Polymer Solar Cells with DIO Additive.

We study the ultrafast photoexcitation dynamics in PBDTTT-C-T (P51, poly(4,8-bis(5-(2-ethylhexyl)-thiophene-2-yl)-benzo[1,2-b:4,5-b']dithiophene-alt-alkylcarbonyl-thieno[3,4-b]thiophene)) film (~100 nm thickness) and PBDTTT-C-T:PC71BM (P51:PC71BM, phenyl-C71-butyric-acid-methyl ester) nanostructured blend (∼100 nm thickness) with/without DIO(1,8-diiodooctane) additives with sub-10 fs transient absorption (TA). It is revealed that hot-exciton dissociation and vibrational relaxation could occur in P51 with a lifetime of ~160 fs and was hardly affected by DIO. However, the introduction of DIO in P51 brings a longer lifetime of polaron pairs, which could make a contribution to photocarrier generation. In P51:PC71BM nanostructured blends, DIO could promote the Charge Transfer (CT) excitons and free charges generation with a ~5% increasement in ~100 fs. Moreover, the dissociation of CT excitons is faster with DIO, showing a ~5% growth within 1 ps. The promotion of CT excitons and free charge generation by DIO additive is closely related with active layer nanomorphology, accounting for Jsc enhancement. These results reveal the effect of DIO on carrier generation and separation, providing an effective route to improve the efficiency of nanoscale polymer solar cells.