Probing photocarrier dynamics of pressurized graphene using time-resolved terahertz spectroscopy

Graphene hosts intriguing photocarrier dynamics such as negative transient terahertz(THz) photoconductivity, high electron temperature, benefiting from the unique linear Dirac dispersion. In this work, the pressure effects of photocarrier dynamics of graphene have been investigated using in situ time-resolved THz spectroscopy in combination with diamond anvil cell exceeding 9 GPa. We find that the negative THz conductivity maintains in our studied pressure range both for monolayer and bilayer graphene. In particular, the amplitude of THz photoconductivity in monolayer graphene manifests an extraordinary dropping with pressure, compared with that from the counterparts such as bulk silicon and bilayer graphene.Concomitantly, the time constant is reduced with increasing pressure, highlighting the pressure-induced hot carrier cooling.The pressure dependence of photocarrier dynamics in monolayer graphene is likely related with the enhancement of the interfacial coupling between diamond surface and sample, allowing for the activity of new electron–phonon scattering. Our work is expected to provide an impetus for the studies of high-pressure THz spectroscopy of two-dimensional materials.

Atomically precise metal-chalcogenide semiconductor molecular nanoclusters with high dispersibility:Designed synthesis and intracluster photocarrier dynamics

A comprehensive understanding of excited-state dynamics of semiconductor quantum dots or nanomaterials at the atomic or molecular level is of scientific importance.Pure inorganic(or non-covalently protected)seimiconductor molecular nanoclusters with atomically precise structure are contributive to establish accurate correlation of excited-state dynamics with their composition/structure,however,the related studies are almost blank because of unresolved solvent dispersion issue.Herein,we designedly created the largest discrete chalcogenide seimiconductor molecular nanoclusters(denoted P2-CuMSnS,M=In or/and Ga)with great dispersibility,and revealed an interesting intracluster“core–shell”charge transfer relaxation dynamics.A systematic red shift in absorption spectra with the gradual substitution of In by Ga was experimentally and computationally investigated,and femtosecond transient absorption measurements further manifested there were three ultrafast processes in excited-state dynamics of P2 nanoclusters with the corresponding amplitudes directed by composition variation.Current results hold the great promise of the solution-processible applications of semiconductor-NC-based quantum dots and facilitate the development of atomically precise nano-chemistry.

Salt-assisted growth and ultrafast photocarrier dynamics of large-sized monolayer ReSe2

Owing to its anisotropic optical and electrical properties,rhenium diselenide(ReSe2)has garnered considerable attention recently as a candidate material for polarization-sensitive photodetectors.However,the direct and controllable synthesis of large-sized ReSe2 with a uniform thickness is still a great challenge.Herein,we have refined the synthesis method to obtain uniform monolayer ReSe2 flakes with a size of up to^106μm on sapphire via an ambient-pressure chemical vapor deposition technique using Na promoter from sodium chloride.Interestingly,optical pump-probe spectroscopy revealed a fast switching from saturable absorption(SA)to absorption enhancement(AE)in subpicosecond time scale,followed by a slower decay induced by exciton recombination.Furthermore,both AE and SA signals exhibited clear angular dependence with a periodicity of 180°,which reflected the dichroism in nonlinear absorption dynamics.In addition,the photocarrier dynamics including free-carrier transport and subpicosecond relaxation due to exciton formation or surface trapping was probed using time resolved terahertz spectroscopy.We believe that our study serves as a reference for atomically controlled synthesis of large-sized ReSe2 and provides useful insights on its optoelectronic properties for novel device applications.