Organic-inorganic perovskites are a class of solution-processed semiconductors holding promise for the realization of low-cost efficient solar cells and on-chip lasers. Despite the recent attention they have attracted, fundamental aspects of the photophysics underlying device operation still remain elusive. Here we use photoluminescence and transmission spectroscopy to show that photoexcitations give rise to a conducting plasma of unbound but Coulomb-correlated electron-hole pairs at all excitations of interest for light-energy conversion and stimulated optical amplification. The conductive nature of the photoexcited plasma has crucial consequences for perovskite-based devices: in solar cells, it ensures efficient charge separation and ambipolar transport while, concerning lasing, it provides a low threshold for light amplification and justifies a favourable outlook for the demonstration of an electrically driven laser. We find a significant trap density, whose cross-section for carrier capture is however low, yielding a minor impact on device performance.
In the last years, high-resolution time tagging has emerged as a promising tool to tackle the problem of high-track density in the detectors of the next generation of experiments at particle colliders. Time resolutions below 50 ps and event average repetition rates of tens of MHz on sensor pixels having a pitch of 50 μm are typical minimum requirements. This poses an important scientific and technological challenge on the development of particle sensors and processing electronics. The TIMESPOT initiative (which stands for TIME and SPace real-time Operating Tracker) aims at the development of a full prototype detection system suitable for the particle trackers of the next-to-come particle physics experiments. This paper describes the results obtained on the first batch of TIMESPOT silicon sensors, based on a novel 3D MEMS (micro electro-mechanical systems) design. We demonstrate that following this approach, the performance of other ongoing silicon sensor developments can be matched and overcome. In addition, 3D technology has already been proved to be robust against radiation damage. A time resolution of the order of 20 ps has been measured at room temperature suggesting also possible improvements after further optimisations of the front-end electronics processing stage.
Intensity instabilities are a common trademark of the photoluminescence of nanoemitters. This general behavior is commonly attributed to random fluctuations of free charges and activation of charge traps reducing the emission yield intermittently. However, the actual physical origin of this phenomenon is actively debated. Here we devise an experiment, variable pulse rate photoluminescence, to control the accumulation of charges and the activation of charge traps. The dynamics of these states is studied, with pulse repetition frequencies from the single-pulse to the megahertz regime, by monitoring photoluminescence spectrograms with picosecond temporal resolution. We find that both photocharging and charge trapping contribute to photoluminescence quenching, and both processes can be reversibly induced by light. Our spectroscopic technique demonstrates that charge accumulation and trap formation are strongly sensitive to the environment, showing different dynamics when nanocrystals are dispersed in solution or deposited as a film.
Room temperature optically pumped lasing is achieved for a new n-type molecular crystal of 2,5-bis(4′-cyanobiphenyl-4-yl)thiophene (BP1T-CN). Efficient stimulated emission in the Fabry–Pérot crystal cavity is supported with a high group refractive index (4.18–4.98), Q factor (910–1860), material gain coefficient (120 cm-1), and a high stimulated emission rate demonstrated by pump–probe measurements
Among solution-processed nanocrystals containing environmentally benign elements, bismuth sulfi de (Bi 2 S 3 ) is a very promising n-type semiconductor for solar energy conversion. Despite the prompt success in the fabrication of optoelectronic devices deploying Bi 2 S 3 nanocrystals, the limited understanding of electronic properties represents a hurdle for further materials developments. Here, two key materials science issues for light-energy conversion are addressed: bandgap tunability via the quantum size effect, and photocarrier trapping. Nanocrystals are synthesized with controlled sizes varying from 3 to 30 nm. In this size range, bandgap tunability is found to be very small, a few tens of meV. First principles calculations show that a useful blueshift, in the range of hundreds of meV, is achieved in ultra-small nanocrystals, below 1.5 nm in size. Similar conclusions are envisaged for the class of pnictide chalcogenides with a ribbon-like structure [Pn 4 Ch 6 ] n (Pn = Bi, Sb; Ch = S, Se). Time-resolved differential transmission spectroscopy demonstrates that only photoexcited holes are quickly captured by intragap states. Photoexcitation dynamics are consistent with the scenario emerging in other metal-chalcogenide nanocrystals: traps are created in metal-rich nanocrystal surfaces by incomplete passivation by long fatty acid ligands. In large nanocrystals, a lower bound to surface trap density of one trap every sixteen Bi 2 S 3 units is found.
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