Many potential applications of monolayer transition metal dichalcogenides (TMDs) require both high photoluminescence (PL) yield and high electrical mobilities. However, the PL yield of as prepared TMD monolayers is low and believed to be limited by defect sites and uncontrolled doping. This has led to a large effort to develop chemical passivation methods to improve PL and mobilities. The most successful of these treatments is based on the nonoxidizing organic “superacid” bis(trifluoromethane)sulfonimide (TFSI) which has been shown to yield bright monolayers of molybdenum disulfide (MoS2) and tungsten disulfide (WS2) but with trap-limited PL dynamics and no significant improvements in field effect mobilities. Here, using steady-state and time-resolved PL microscopy we demonstrate that treatment of WS2 monolayers with oleic acid (OA) can greatly enhance the PL yield, resulting in bright neutral exciton emission comparable to TFSI treated monolayers. At high excitation densities, the OA treatment allows for bright trion emission, which has not been demonstrated with previous chemical treatments. We show that unlike the TFSI treatment, the OA yields PL dynamics that are largely trap free. In addition, field effect transistors show an increase in mobilities with the OA treatment. These results suggest that OA serves to passivate defect sites in the WS2 monolayers in a manner akin to the passivation of colloidal quantum dots with OA ligands. Our results open up a new pathway to passivate and tune defects in monolayer TMDs using simple “wet” chemistry techniques, allowing for trap-free electronic properties and bright neutral exciton and trion emission.

We present a novel optical transient absorption and reflection microscope based on a diffraction-limited pump pulse in combination with a wide-field probe pulse, for the spatiotemporal investigation of ultrafast population transport in thin films. The microscope achieves a temporal resolution down to 12 fs and simultaneously provides sub-10 nm spatial accuracy. We demonstrate the capabilities of the microscope by revealing an ultrafast excited-state exciton population transport of up to 32 nm in a thin film of pentacene and by tracking the carrier motion in p-doped silicon. The use of few-cycle optical excitation pulses enables impulsive stimulated Raman microspectroscopy, which is used for in situ verification of the chemical identity in the 100–2000 cm–1 spectral window. Our methodology bridges the gap between optical microscopy and spectroscopy, allowing for the study of ultrafast transport properties down to the nanometer length scale.

Heterostructures of two-dimensional (2D) transition metal dichalcogenides (TMDs) and inorganic semiconducting zero-dimensional (0D) quantum dots (QDs) offer unique charge and energy transfer pathways which could form the basis of novel optoelectronic devices. To date, most has focused on charge transfer and energy transfer from QDs to TMDs, i.e. from 0D to 2D. Here, we present a study of the energy transfer process from a 2D to 0D material, specifically exploring energy transfer from monolayer tungsten disulphide (WS2) to near infrared (NIR) emitting lead sulphide-cadmium sulphide (PbS-CdS) QDs. The high absorption cross section of WS2 in the visible region combined with the potentially high photoluminescence (PL) efficiency of PbS QD systems, make this an interesting donoracceptor system that can effectively use the WS2 as an antenna and the QD as a tuneable emitter, in this case downshifting the emission energy over hundreds of meV. We study the energy transfer process using photoluminescence excitation (PLE) and PL microscopy, and show that 58% of the QD PL arises due to energy transfer from the WS2. Time resolved photoluminescence (TRPL) microscopy studies show that the energy transfer process is faster than the intrinsic PL quenching by trap states in the WS2, thus allowing for efficient energy transfer. Our results establish that QDs could be used as tuneable and high PL efficiency emitters to modify the emission properties of TMDs. Such TMD/QD heterostructures could have applications in light emitting technologies, artificial light harvesting systems or be used to read out the state of TMD devices optically in various logic and computing applications

The inherently low photoluminescence (PL) yields in as prepared transition metal dichalcogenide (TMD) monolayers are broadly accepted to be the result of atomic vacancies (i.e. defects) and uncontrolled doping, which...

Luminescent colloidal CdSe nanorings are a new type of semiconductor structure that have attracted interest due to the potential for unique physics arising from their non-trivial toroidal shape. However, the exciton properties and dynamics of these materials with complex topology are not yet well understood. Here, we use a combination of femtosecond vibrational spectroscopy, temperature-resolved photoluminescence (PL), and single particle measurements to study these materials. We find that on transformation of CdSe nanoplatelets to nanorings, by perforating the center of platelets, the emission lifetime decreases and the emission spectrum broadens due to ensemble variations in the ring size and thickness. The reduced PL quantum yield of nanorings (~10%) compared to platelets (~30%) is attributed to an enhanced coupling between: (i) excitons and CdSe LO-phonons at 200 cm -1 and (ii) negatively charged selenium-rich traps which give nanorings a high surface charge (~-50 mV).Population of these weakly emissive trap sites dominates the emission properties with an increased trap emission at low temperatures relative to excitonic emission. Our results provide a detailed picture of the nature of excitons in nanorings and the influence of phonons and surface charge in explaining the broad shape of the PL spectrum and the origin of PL quantum yield losses. Furthermore, they suggest that the excitonic properties of nanorings are not solely a consequence of the toroidal shape but are also a result of traps introduced by puncturing the platelet center.