Photoelectron angular distribution studies for two spin\u2013orbit-split components of Xe 3d subshell: a critical comparison between theory and experiment

The photoelectron angular distribution asymmetry parameters \u3b2 of the Xe 3d subshell were investigated using an x-ray free-electron laser (XFEL) at photon energies of 750 and 800 eV. Owing to the perfect polarization of the XFEL and two-dimensional momentum imaging capability of our velocity map imaging spectrometer, we determined the \u3b2 values with high accuracy. The \u3b2 values were also investigated based on relativistic time-dependent density functional theory calculations of up to 900 eV of photon energies. By comparing all the available experimental results including our data with the most reliable theories on the photon energy dependence of the \u3b2 parameters, serious differences are noted between the experiments and theories. Further studies on resolving this difference will provide new insight into the photoionization processes of the deep inner shells

Slow hot carrier cooling in cesium lead iodide perovskites

Lead halide perovskites are attracting a great deal of interest for optoelectronic applications such as solar cells, LEDs, and lasers because of their unique properties. In solar cells, heat dissipation by hot carriers results in a major energy loss channel responsible for the Shockley–Queisser efficiency limit. Hot carrier solar cells offer the possibility to overcome this limit and achieve energy conversion efficiency as high as 66% by extracting hot carriers. Therefore, fundamental studies on hot carrier relaxation dynamics in lead halide perovskites are important. Here, we elucidated the hot carrier cooling dynamics in all-inorganic cesium lead iodide (CsPbI3) perovskite using transient absorption spectroscopy. We observe that the hot carrier cooling rate in CsPbI3 decreases as the fluence of the pump light increases and the cooling is as slow as a few 10 ps when the photoexcited carrier density is 7 × 1018 cm−3, which is attributed to phonon bottleneck for high photoexcited carrier densities. Our findings suggest that CsPbI3 has a potential for hot carrier solar cell applications

Investigation of Interfacial Charge Transfer in Solution Processed Cs2SnI6 Thin Films

Cesium tin halide based perovskite Cs2SnI6 has been subjected to in-depth investigations owing to its potentiality toward the realization of environment benign Pb free and stable solar cells. In spite of the fact that Cs2SnI6 has been successfully utilized as an efficient hole transport material owing to its p-type semiconducting nature, however, the nature of the majority carrier is still under debate. Therefore, intrinsic properties of Cs2SnI6 have been investigated in detail to explore its potentiality as light absorber along with facile electron and hole transport. A high absorption coefficient (5 × 104 cm–1) at 700 nm indicates the penetration depth of 700 nm light to be 0.2 μm, which is comparable to conventional Pb based solar cells. Preparation of pure and CsI impurity free dense thin films with controllable thicknesses of Cs2SnI6 by the solution processable method has been reported to be difficult owing to its poor solubility. An amicable solution to circumvent such problems of Cs2SnI6 has been provided utilizing spray-coating in combination with spin-coating. The presence of two emission peaks at 710 and 885 nm in the prepared Cs2SnI6 thin films indicated coexistence of quantum dot and bulk parts which were further supported by transmission electron microscopy (TEM) investigations. Time-resolved photoluminescence (PL) and transient absorption spectroscopy (TAS) were employed to investigate the excitation carrier lifetime, which revealed fast decay kinetics in the picoseconds (ps) to nanoseconds (ns) time domains. Time-resolved microwave photoconductivity decay (MPCD) measurement provided the mobile charge carrier lifetime exceeding 300 ns, which was also in agreement with the nanosecond transient absorption spectroscopy (ns-TAS) indicating slow charge decay lasting up to 20 μs. TA assisted interfacial charge transfer investigations utilizing Cs2SnI6 in combination with n-type PCBM and p-type P3HT exhibited both intrinsic electron and hole transport

Ultrafast Electron Injection from Photoexcited Perovskite CsPbI3 QDs into TiO2 Nanoparticles with Injection Efficiency near 99%

Photoexcited electron injection dynamics from CsPbI3 quantum dots (QDs) to wide gap metal oxides are studied by transient absorption spectroscopy. Experimental results show under a low excitation intensity that ∼99% of the photoexcited electrons in CsPbI3 QDs can be injected into TiO2 with a size-dependent rate ranging from 1.30 × 1010 to 2.10 × 1010 s–1, which is also ∼2.5 times faster than that in the case of ZnO. A demonstration QD-sensitized solar cell based on a CsPbI3/TiO2 electrode is fabricated that delivers a power conversion efficiency of 5%

Colloidal Synthesis of Air-Stable Alloyed CsSn1–xPbxI3 Perovskite Nanocrystals for Use in Solar Cells

Organic–inorganic hybrid perovskite solar cells have demonstrated unprecedented high power conversion efficiencies in the past few years. Now, the universal instability of the perovskites has become the main barrier for this kind of solar cells to realize commercialization. This situation can be even worse for those tin-based perovskites, especially for CsSnI3, because upon exposure to ambient atmosphere the desired black orthorhombic phase CsSnI3 would promptly lose single crystallinity and degrade to the inactive yellow phase, followed by irreversible oxidation into metallic Cs2SnI6. By alloying CsSnI3 with CsPbI3, we herein report the synthesis of alloyed perovskite quantum dot (QD), CsSn1–xPbxI3, which not only can be phase-stable for months in purified colloidal solution but also remains intact even directly exposed to ambient air, far superior to both of its parent CsSnI3 and CsPbI3 QDs. Ultrafast transient absorption spectroscopy studies reveal that the photoexcited electrons in the alloyed QDs can be injected into TiO2 nanocrystals at a fast rate of 1.12 × 1011 s–1, which enables a high photocurrent generation in solar cells

Electronic States of Cobalt Cluster Cations : Absorption Spectrum of d Electrons and Spin-polarized DV-Xα Calculation

Photodissociation spectra of cobalt cluster ion-argon atom complexes, Co^+_nAr (n=3-5), were measured by detecting the product ions Co^+_n and Co^+_, with a tunable laser pulse from an optical parametric oscillator in the photon-energy range from 0.7 to 2.8 eV. The photodissociation spectra thus obtained are equivalent to the optical absorption spectra of the underlying cobalt cluster ions, Co^+_n, because the argon atom is weakly bound to Co^+_n. The spectrum was analyzed by means of a spin-polarized DV-Xα calculation, and the electronic and the geometric structures of Co^+_3 and Co^+_4 were determined. The analysis shows that all the transitions in the entire energy range studied occur between occupied and unoccupied energy levels associated with 3d atomic orbitals (AOs) having the minority spin. The spin difference (difference in population per Co atom between the majority and the minority spins) was evaluated from the electronic structures thus obtained. The spin differences of 2.00 for Co^+_3 and 1.75 for Co^+_4 indicate ferromagnetic spin coupling in these cobalt cluster ions

Development of a plasma shutter applicable to 100-mJ-class, 10-ns laser pulses and the characterization of its performance

© 2019 Optical Society of America.For the purpose of preparing a sample of aligned and oriented molecules in the laser-field-free condition, we developed a plasma shutter, which enables laser pulses with 100-mJ-class, 10-ns pulse durations to be rapidly turned off within ∼150 fs. In this work, the residual field intensity after the rapid turn off is carefully examined by applying the shaped laser pulse to OCS molecules in the rotational ground state. Based on the comparison between the observation of alignment revivals of the OCS molecules and the results of numerical simulations, we demonstrate that the residual field intensity is actually negligible (below 0.4% of the peak intensity) and, if any, does not influence the alignment and orientation dynamics at al