Ultrafast Electron and Hole Transfer and Efficient Charge Separation in a Sb2Se3/CdS Thin Film p-n Heterojunction.

Harvesting solar energy for different applications requires the continuous development of new semiconducting materials to exploit a broad part of the solar spectrum. In this direction, antimony selenide (Sb2Se3) has attracted a tremendous amount of attention over the past few years as a light-harvesting material for photovoltaic device applications owing to its phase stability, high absorption coefficient, earth abundance, and low toxicity. Here, we have fabricated a high-quality heterojunction of a p-type Sb2Se3 film and an n-type CdS film using the thermal evaporation technique. The photocurrent of the heterosystem was significantly higher than that of the pristine materials. This optoelectronic response was investigated using femtosecond transient absorption (TA) spectroscopy. TA study reveals the existence of an instantaneous electron transfer from Sb2Se3 to CdS, accompanied by a substantial charge separation at the heterojunction. Our study deals with the investigation of a well-designed p-n device, paving the way for the fabrication of highly efficient photovoltaic devices.

Ultrafast Hole Migration at the p-n Heterojunction of One-Dimensional SnS Nanorods and Zero-Dimensional CdS Quantum Dots.

The p-n heterojunctions fabricated from one-dimensional (1D) p-type tin sulfide nanorods (SnS NRs) decorated with n-type zero-dimensional (0D) cadmium sulfide quantum dots (CdS QDs) have gained significant research attention in energy storage devices. Herein, we have successfully synthesized a 1D/0D SnS@CdS heterostructure (HS) using a hot injection method. Structural and morphological studies clearly suggest that CdS QDs are uniformly anchored on the surface of SnS NRs, resulting in intimate contact between two components. The photoluminescence (PL) study revealed the transfer of photoexcited holes from CdS QDs to SnS NRs, which was further confirmed by transient absorption (TA) studies. TA measurements demonstrate the hole transfer from the valence band of CdS QDs to SnS NRs and delocalization of electrons between the conduction band of SnS NRs and CdS QDs in SnS@CdS HS, resulting in efficient charge separation across the p-n heterojunction. These findings will open up a new paradigm for improving the efficiency of optoelectronic devices.

Temperature driven charge transfer process in quantum confined two-dimensional Mn-doped CsPbBr3 perovskite nanoplatelets.

A temperature dependent transient absorption study has been demonstrated for Mn2+ doped CsPbBr3 nanoplatelets. At 5 K, charge transfer is suppressed due to the trapping of charge carriers in defect states. By contrast, at 300 K, an efficient charge/energy transfer process is observed as the thermally active carriers become de-trapped from the defect states upon strong exciton-phonon coupling.

Probing the charge transfer mechanisms in type-II Cs2AgBiBr6-CdSe composite system: ultrafast insights.

Lead-free halide-based double perovskites (DPs) have established themselves as the emerging nontoxic alternatives for photovoltaic (PV) applications thus substituting the long-standing lead halide perovskites. Among the prospective lead-free DPs, Cs2AgBiBr6has gained immense popularity owing to the fascinating properties demonstrated by them including low carrier effective mass and microsecond lifetime for electron-hole recombination. Nevertheless, the large, indirect bandgap remains the prime hurdle that restrains commercialization of the Cs2AgBiBr6DPs based PV devices. A rational solution could be designing its heterostructure with another suitable material that could mitigate the inadequacies of Cs2AgBiBr6DPs. With this line of thought, herein we synthesized a composite of Cs2AgBiBr6DPs with CdSe NCs and then performed transient absorption (TA) spectroscopic measurements to introspect its photophysical aspects. Executing excitation energy-dependent studies clearly reveal the carrier transfer efficiency to be strongly pump-dependent. Upon exciting with 350 nm pump, in compliance with the energy band alignment and tendency of both the constituents to be photoexcited across their bandgap, there is a bidirectional transfer of hot electrons anticipated in the composite system. Nevertheless, the TA outcomes indicate the transfer of hot electrons from CdSe to Cs2AgBiBr6to be more favorable out of the bidirectional pathways. Employing further lower pump energies (480 nm) when only CdSe NCs are capable of being excited, the transfer efficiency of the electrons from CdSe to Cs2AgBiBr6is noticed to be fairly low. Besides this, when the pump wavelength is tuned to 530 nm i.e. quite close to the CdSe band edge, no electron transfer is noticeable despite the anticipation from thermodynamic feasibility. Thus, as reflected by the TA kinetics, electron transfer is discerned to be more efficient from the hot states rather than the band edges. Most advantageously, charge separation is successfully achieved in this never explored composite architecture which eases the carrier extraction and minimizes the otherwise prevalent fast recombination processes.

Defect-Interceded Cascading Energy Transfer and Underlying Charge Transfer in Europium-Doped CsPbCl3 Nanocrystals.

Rare-earth ion (RE3+) doping in cesium lead chloride (CsPbCl3) has unlocked novel prospects to explore changes in optical, magnetic, and charge carrier transport properties. This leads to a huge advancement in optoelectronic applications, yet deep understanding of the photophysics governing the energy transfer processes is lacking and demands vital attention. Herein, we probe into the mechanistic transfer processes from the band edge of the host (CsPbCl3) to the dopant europium ion (Eu3+) with the aid of femtosecond fluorescence upconversion and transient absorption (TA) spectroscopy. The upconversion measurement portrays a defect-mediated cascading energy transfer from CsPbCl3 to Eu3+ and further cross-relaxation among Eu3+ states. Moreover, TA studies reveal that there is charge transfer from the band edge of CsPbCl3 to doping-induced shallow defect states. Furthermore, two-photon absorption study establishes no compromise in the transfer mechanism even upon bandgap excitation. This work validates that Eu-CsPbCl3 is an apt entrant for optoelectronic applications.