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Register a new userEffect of Dimensionality on the Optical Absorption Properties of CsPbI$_3$ Perovskite Nanocrystals
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The band-gaps of CsPbI$_3$ perovskite nanocrystals are measured by absorption spectroscopy at cryogenic temperatures. Anomalous band-gap shifts are observed in CsPbI$_3$ nanocubes and nanoplatelets, which are modeled accurately by band-gap renormalization due to lattice vibrational modes. We find that decreasing dimensionality of the CsPbI$_3$ lattice in nanoplatelets greatly reduces electron-phonon coupling, and dominant out-of-plane quantum confinement results in a homogeneously broadened absorption lineshape down to cryogenic temperatures. An absorption tail forms at low-temperatures in CsPbI$_3$ nanocubes, which we attribute to shallow defect states positioned near the valence band-edge.
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Previous theoretical calculations show azetidinium has the right radial size to form a 3D perovskite with lead halides [1], and has been shown to impart, as the A-site cation of ABX3 unit, beneficial properties to ferroelectric perovskites [2]. However, there has been very limited research into its use as the cation in lead halide perovskites to date. In this communication we report the synthesis and characterization of azetidinium-based lead mixed halide perovskite colloidal nanocrystals. The mixed halide system is iodine and chlorine unlike other reported nanocrystals in the literature where the halide systems are either iodine/bromine or bromine/chlorine. UV-visible absorbance data, complemented with photoluminescence spectroscopy, reveals an indirect-bandgap of about 1.96 eV for our nanocrystals. Structural characterization using TEM shows two distinct interatomic distances (2.98 +/- 0.15 Angstroms and 3.43 +/- 0.16 Angstroms) and non-orthogonal lattice angles (approximately 112 degrees) intrinsic to the nanocrystals with a probable triclinic structure revealed by XRD. The presence of chlorine and iodine within the nanocrystals is confirmed by EDS spectroscopy. Finally, light-induced electron paramagnetic resonance (LEPR) spectroscopy with PCBM confirms the photoinduced charge transfer capabilities of the nanocrystals. The formation of such semiconducting lead mixed halide perovskite using azetidinium as the cation suggests a promising subclass of hybrid perovskites holding potential for optoelectronic applications such as in solar cells and photodetectors.
We report on the study of optical properties of mist CVD grown alpha Gallium oxide with the observation of excitonic absorption in spectral responsivity measurements. 163 nm of Gallium oxide was grown on sapphire using Gallium acetylacetonate as the starting solution at a substrate temperature of 450 deg C. The film was found to be crystalline and of alpha phase with an on axis full width at half maximum of 92 arcsec as confirmed from X ray diffraction scans. The Taucs plot extracted from absorption spectroscopy exhibited two transitions in the UV regime at 5.3 eV and 5.6 eV, corresponding to excitonic absorption and direct band to band transition respectively. The binding energy of exciton was extracted to be 114 meV from spectral responsivity measurements. Further, metal semiconductor metal photodetectors with lateral inter digitated geometry were fabricated on the film. A sharp band edge was observed at 230 nm in the spectral response with peak responsivity of around 1 Amperes per Watt at a bias of 20 V. The UV to visible rejection ratio was found to be around 100 while the dark current was measured to be around 0.1 nA.
Dark ground state exciton in semiconductor nanocrystals has been a subject of much interest due to its long lifetime attractive for applications requiring long-lived electronic or spin states. Significant effort has been made recently to explore and access the dark exciton level in metal halide perovskite nanocrystals, which are emerging as a superior source of photons and charges compared to other existing semiconductor nanocrystals. However, the direct observation of long-lived photoluminescence from dark exciton has remained elusive in metal halide perovskite nanocrystals. Here, we report the observation of the intense emission from dark ground state exciton with 1-10 us lifetime in strongly quantum confined CsPbBr3 nanocrystals, which contrasts the behavior of weakly confined system explored so far. The study in CsPbBr3 nanocrystals with varying degree of confinement has revealed the crucial role of quantum confinement in enhancing the bright-dark exciton level splitting which is important for accessing the dark exciton. Our work demonstrates the future potential of strongly quantum-confined perovskite nanocrystals as a new platform to utilize dark excitons.
$beta$-Ga$_2$O$_3$ is an ultra-wide bandgap semiconductor and is thus expected to be optically transparent to light of sub-bandgap wavelengths well into the ultraviolet. Contrary to this expectation, it is found here that free electrons in n-doped $beta$-Ga$_2$O$_3$ absorb light from the IR to the UV wavelength range via intra- and inter-conduction band optical transitions. Intra-conduction band absorption occurs via an indirect optical phonon mediated process with a $1/omega^{3}$ dependence in the visible to near-IR wavelength range. This frequency dependence markedly differs from the $1/omega^{2}$ dependence predicted by the Drude model of free-carrier absorption. The inter-conduction band absorption between the lowest conduction band and a higher conduction band occurs via a direct optical process at $lambda sim 349$ nm (3.55 eV). Steady state and ultrafast optical spectroscopy measurements unambiguously identify both these absorption processes and enable quantitative measurements of the inter-conduction band energy, and the frequency dependence of absorption. Whereas the intra-conduction band absorption does not depend on light polarization, inter-conduction band absorption is found to be strongly polarization dependent. The experimental observations, in excellent agreement with recent theoretical predictions for $beta$-Ga$_2$O$_3$, provide important limits of sub-bandgap transparency for optoelectronics in the deep-UV to visible wavelength range, and are also of importance for high electric field transport effects in this emerging semiconductor.
The dynamical and static Rashba effects in hybrid methylammonium (MA) lead halide perovskites have recently been theoretically predicted. However, only the static effect was experimentally confirmed so far. Here we report on the dynamical Rashba effect observed using snapshot transient absorption spectral imaging with 400 nm pumping for a fully encapsulated film of 20-nm-sized 3D MAPbBr3 nanocrystals. The effect causes a 240 meV splitting of the lowest-energy absorption bleaching band, initially appearing over sub-ps timescale and progressively stabilizing to 60 meV during 500 ps. The integrated intensities of the split subbands demonstrate a photon-helicity-dependent asymmetry, thus proving the Rashba-type splitting and providing direct experimental evidence for the Rashba spin-split edge states in lead halide perovskite materials. The ultrafast dynamics is governed by the relaxation of two-photon-excited electrons in the Rashba spin-split system caused by a built-in electric field originating from dynamical charge separation in the entire MAPbBr3 nanocrystal.
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