Low-temperature luminescence in organic-inorganic lead iodide perovskite single crystals

We present temperature and laser-power dependent photoluminescence (PL) study of methylammonium lead iodide (CH3NH3PbI3) single crystals in the orthorhombic phase. At temperatures below 140 K, we revealed the multi-component PL emission. In addition to a free exciton with an energy of 1.65 eV, we found emission bands with peaks approximately equal to 1.6 eV, 1.52 eV, and 1.48 eV. Analysis of the thermal evolution of the intensities, peak positions, and linewidths of all the PL bands allowed one to determine their origin. We attributed the PL peak with the energy of 1.6 eV to a bound exciton, while the free exciton-bound exciton splitting energy is 50-60 meV. The PL emission with an energy of 1.52 eV can be explained by the donor-acceptor pair (DAP) recombination, where donor and acceptor defects have a depth of about 12 meV and 120 meV, respectively. MA (CH3NH3) interstitials (MA+i ) and lead vacancies (V2-Pb) are the most suitable for the DAP transition to occur in CH3NH3PbI3 crystals. The 1.48 eV PL emission is consistent with the recombination of self-trapped excitons, and interstitial iodine is likely to be an active trap source. We found the variation of the self-trapped depth from 15 meV (at T<80 K) to 53 meV (at T>80 K) with increasing the temperature. Although the multi-component PL emission in CH3NH3PbI3 single crystals appears at low temperatures, defects and excitonic traps that cause this emission can affect the photophysics of hybrid perovskites at higher temperatures.

Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors

Strong-coupling between excitons and confined photonic modes can lead to the formation of new quasi-particles termed exciton-polaritons which can display a range of interesting properties such as super-fluidity, ultrafast transport and Bose-Einstein condensation. Strong-coupling typically occurs when an excitonic material is confided in a dielectric or plasmonic microcavity. Here, we show polaritons can form at room temperature in a range of chemically diverse, organic semiconductor thin films, despite the absence of an external cavity. We find evidence of strong light-matter coupling via angle-dependent peak splittings in the reflectivity spectra of the materials and emission from collective polariton states. We additionally show exciton-polaritons are the primary photoexcitation in these organic materials by directly imaging their ultrafast (5 × 106 m s−1), ultralong (~270 nm) transport. These results open-up new fundamental physics and could enable a new generation of organic optoelectronic and light harvesting devices based on cavity-free exciton-polaritons

Trap-free exciton dynamics in monolayer WS2 via oleic acid passivation

Two-dimensional transition metal dichalcogenides have attracted tremendous attention in the past few decades due to their attractive optoelectronic properties. However, their widespread utility in photonic devices and components is still...

High-efficiency Wavelength Tunable Monolayer LED with Hybrid Continuous-pulsed Injection

High-efficiency and wavelength-tunable light emitting diode (LED) devices will play an important role in future advanced optoelectronic systems. Traditional semiconductor LED devices typically have a fixed emission wavelength that is determined by the energy of the emission states. Here, we developed a novel high-efficiency and wavelength-tunable monolayer WS2 LED device, which operates in the hybrid mode of continuous-pulsed injection. This hybrid injection enables highly enhanced emission efficiency (> 20 times) and the effective size of emission area (> 5 times) at room temperature. The emission wavelength of WS2 monolayer LED device can be tuned over more than 40 nm by driving AC voltages, from exciton emission to trion emission, and further to defect emissions. The quantum efficiency of defect electroluminescence (EL) emission is measured to be more than 24.5 times larger than that from free exciton and trion EL emissions. The separate carrier injection in our LED also demonstrate advantage in allowing to visualize and distinguish defect species in real space. Those defects are assigned to be negatively charged defects. Our results open a new route to develop high-performance and wavelength-tunable LED devices for future advanced optoelectronic applications.

Anisotropic optical properties of single Si2Te3 nanoplates

We report a combined experimental and computational study of the optical properties of individual silicon telluride (Si2Te3) nanoplates. The p-type semiconductor Si2Te3 has a unique layered crystal structure with hexagonal closed-packed Te sublattices and Si–Si dimers occupying octahedral intercalation sites. The orientation of the silicon dimers leads to unique optical and electronic properties. Two-dimensional Si2Te3 nanoplates with thicknesses of hundreds of nanometers and lateral sizes of tens of micrometers are synthesized by a chemical vapor deposition technique. At temperatures below 150 K, the Si2Te3 nanoplates exhibit a direct band structure with a band gap energy of 2.394 eV at 7 K and an estimated free exciton binding energy of 150 meV. Polarized reflection measurements at different temperatures show anisotropy in the absorption coefficient due to an anisotropic orientation of the silicon dimers, which is in excellent agreement with theoretical calculations of the dielectric functions. Polarized Raman measurements of single Si2Te3 nanoplates at different temperatures reveal various vibrational modes, which agree with density functional perturbation theory calculations. The unique structural and optical properties of nanostructured Si2Te3 hold great potential applications in optoelectronics and chemical sensing.

Carrier Transfer and Capture Kinetics of the TiO2/Ag2V4O11 Photocatalyst

In this paper, TiO2/Ag2V4O11 nanoheterojunctions have been synthesized by hydrothermal methods, which show enhanced photocatalytic activity compared to TiO2 under visible light. Moreover, the TiO2/Ag2V4O11 nanoheterojunction with set molar ratio of 2:1, referred to as TA2, show the highest visible light photocatalytic activity, which could decompose about 100% RhB molecules within 80 min of irradiation with visible light. Specially, the time-resolved photoluminescence spectrum of TA2 demonstrates that the free exciton recombination occurs in approximately 1.7 ns, and the time scale for Shockley–Read–Hall recombination of photogenerated electrons and holes is prolonged to 6.84 ns. The prolonged timescale of TA2 compared to TiO2 and Ag2V4O11 can be attributed to the carrier separation between nanojunctions and the carrier capture by interfacial defects. Furthermore, the enhanced photocatalytic activity of TiO2/Ag2V4O11 nanoheterojunctions also benefits from the synergistic effect of the broadened absorption region, higher photocarrier generation, longer carrier lifetime, and quicker collection dynamics.

Investigation of the Role of the Environment on the Photoluminescence and the Exciton Relaxation of CsPbBr3 Nanocrystals Thin Films

In this work, we present a detailed optical investigation of the effects of the environment on the photoluminescence (PL) spectra and the relaxation dynamics of pristine and aged CsPbBr3 nanocrystal (NC) thin films. We demonstrate that, contrary to previous results on similar NCs, the PL intensity of pristine NCs is higher when the sample is in wet air than in vacuum, due to the passivation of defects reducing the free exciton trapping and the bound excitons non-radiative relaxation. The aged NCs show a PL intensity increase in wet air nine times stronger than the pristine ones, due to an interplay between static and dynamic effects, increasing the number of emitting NCs and reducing the non-radiative recombination rate of free excitons. These results improve the understanding of the possible interactions between perovskite NCs and the environment, which could be relevant for the development of optical gas sensors exploiting perovskite NCs.