We
report a colloidal synthesis approach to CsPbBr3 nanoplatelets
(NPLs). The nucleation and growth of the platelets, which takes place
at room temperature, is triggered by the injection of acetone in a
mixture of precursors that would remain unreactive otherwise. The
low growth temperature enables the control of the plate thickness,
which can be precisely tuned from 3 to 5 monolayers. The strong two-dimensional
confinement of the carriers at such small vertical sizes is responsible
for a narrow PL, strong excitonic absorption, and a blue shift of
the optical band gap by more than 0.47 eV compared to that of bulk
CsPbBr3. We also show that the composition of the NPLs
can be varied all the way to CsPbBr3 or CsPbI3 by anion exchange, with preservation of the size and shape of the
starting particles. The blue fluorescent CsPbCl3 NPLs represent
a new member of the scarcely populated group of blue-emitting colloidal
nanocrystals. The exciton dynamics were found to be independent of
the extent of 2D confinement in these platelets, and this was supported
by band structure calculations.
Electron/hole traps related to interstitial iodine defects show the typical features of iodine photo-electrochemistry, inducing MAPbI3 defect tolerance.
Metal halide perovskites have become a popular material system for fabricating photovoltaics and various optoelectronic devices. However, long-term reliability must be assured. Instabilities are manifested as light-induced ion migration and segregation, which can lead to material degradation. Discordant reports have shown a beneficial role of ion migration under illumination, leading to defect healing. By combining ab initio simulations with photoluminescence measurements under controlled conditions, we demonstrate that photo-instabilities are related to light-induced formation and annihilation of defects acting as carrier trap states. We show that these phenomena coexist and compete. In particular, long-living carrier traps related to halide defects trigger photoinduced material transformations, driving both processes. Defect formation can be controlled by blocking under-coordinated surface sites, which act as a defect reservoir. By use of a passivation strategy we are thus able to stabilize the perovskite layer, leading to improved optoelectronic material quality and enhanced photostability in solar cells.
The presence of various types of chemical interactions in metal‐halide perovskite semiconductors gives them a characteristic “soft” fluctuating structure, prone to a wide set of defects. Understanding of the nature of defects and their photochemistry is summarized, which leverages the cooperative action of density functional theory investigations and accurate experimental design. This knowledge is used to describe how defect activity determines the macroscopic properties of the material and related devices. Finally, a discussion of the open questions provides a path towards achieving an educated prediction of device operation, necessary to engineer reliable devices.
A hygroscopic polymer thin film successfully encapsulates an organic–inorganic halide perovskite layer, showing enhanced stability of the solar cell operating in a humid atmosphere.
Experimental section
Sample preparationLead(II) bromide (PbBr 2 , ≥98%), N,N-dimethylformamide (DMF, anhydrous, 99.8%), Chlorobenzene (anhydrous, 99.8%), and dimethyl sulfoxide (DMSO, anhydrous, ≥99.9%) were purchased from Sigma-Aldrich; methylammonium bromide (MABr) and methylammonium iodide (MAI) were purchased from Dyesol; and lead (II) iodide (PbI 2 , 99.9985%, CAS No. 10101-63-0) was purchased from Alfa Aesar. All chemicals were used without any further purification. Glass substrates were cleaned in acetone and isopropyl alcohol (IPA) for 10 minutes by sonication. The cleaned glass substrates were treated with Oxygen plasma for 10 minutes before any further deposition.
We study the nature of photo-excited charge carriers in CsPbBr3 nanocrystal thin films by ultrafast optical pump -THz probe spectroscopy. We observe a deviation from a pure Drude dispersion of the THz dielectric response that is ascribed to the polaronic nature of carriers; a transient blueshift of observed phonon frequencies is indicative of the coupling between photogenerated charges and stretching-bending modes of the deformed inorganic sublattice, as confirmed by DFT calculations.
A large number of graphene molecules, or large polycyclic aromatic hydrocarbons (PAHs), have been synthesized and display various optoelectronic properties. Nevertheless, their potential for application in photonics has remained largely unexplored. Herein, we describe the synthesis of a highly luminescent and stable graphene molecule, namely a substituted dibenzo[hi,st]ovalene (DBO 1), with zigzag edges and elucidate its promising optical‐gain properties by means of ultrafast transient absorption spectroscopy. Upon incorporation of DBO into an inert polystyrene matrix, amplified stimulated emission can be observed with a relatively low power threshold (ca. 60 μJ cm−2), thus highlighting its high potential for lasing applications.
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