CH3NH3PbI3 perovskite layered films deposited on substrates with and without a titania support structure have been prepared and studied using time-resolved femtosecond transient absorption (fs-TA) spectroscopy in the visible light range (450-800 nm). The electron injection dynamics from the photoexcited perovskite layers to the neighboring film structures could be directly monitored via the transient bleaching dynamics of the perovskite at ∼750 nm and thus systematically studied as a function of the layer-by-layer architecture. In addition, for the first time we could spectrally distinguish transient bleaching at ∼750 nm from laser-induced fluorescence that occurs red-shifted at ∼780 nm. We show that an additional bleach feature at ∼510 nm appears when PbI2 is present in the perovskite film. The amplitudes of the PbI2 and perovskite TA peaks were compared to estimate relative amounts of PbI2 in the samples. Kinetic analysis reveals that perovskite films with less PbI2 show faster relaxation rates than those containing more PbI2. These fast dynamics are attributed to charge carrier trapping at perovskite grain boundaries, and the slower dynamics in samples containing PbI2 are due to a passivation effect, in line with other recently reported work.
Reversible control of adhesion is an important feature of many desired, existing, and potential systems, including climbing robots, medical tapes, and stamps for transfer printing. We present experimental and theoretical studies of pressure modulated adhesion between flat, stiff objects and elastomeric surfaces with sharp features of surface relief in optimized geometries. Here, the strength of nonspecific adhesion can be switched by more than three orders of magnitude, from strong to weak, in a reversible fashion. Implementing these concepts in advanced stamps for transfer printing enables versatile modes for deterministic assembly of solid materials in micro/nanostructured forms. Demonstrations in printed two- and three-dimensional collections of silicon platelets and membranes illustrate some capabilities. An unusual type of transistor that incorporates a printed gate electrode, an air gap dielectric, and an aligned array of single walled carbon nanotubes provides a device example.
This letter describes the physics and application of an approach to transfer printing that utilizes targeted shear loading to modulate stamp adhesion in a controlled and repeatable fashion. Experimental measurements of pull-off forces as functions of shear and stamp dimension reveal key scaling properties and provide a means for comparison to theory and modeling. Examples of printed structures in suspended and multilayer configurations demonstrate some capabilities in micro/nanoscale materials assembly.
Temperature-dependent thermal conductivity in the range between 7 and 300 K was measured for CH 3 NH 3 PbI 3 and CsPbI 3 and compared to a Debye model via the Callaway method. Thermal conductivity was found to be extremely low across the whole temperature range for both materials, with CH 3 NH 3 PbI 3 lower than CsPbI 3 . Fitting analysis showed that a resonant phonon scattering term can account for the difference in thermal transport behavior between the perovskite with a methylammonium (MA) ion versus a single cesium atom in the cationic A site of the lattice. The resonant frequency associated with this term is in the range of ∼15−30 cm −1 , pointing to the rotational degree of freedom of the organic ion. Analysis of the temperature dependence of the possible phonon scattering mechanisms showed that thermal conductivity of both CH 3 NH 3 PbI 3 and CsPbI 3 perovskites was dominated by Umklapp scattering at room temperature, and the rotation of the organic cation may be responsible for suppressing the thermal conductivity of CH 3 NH 3 PbI 3 in comparison with CsPbI 3 , particularly at low temperatures, ∼25 K. This work presents the first determination of temperature-dependent thermal conductivity of CsPbI 3 .
In this work, the spatially dependent recombination kinetics of mixed-halide hybrid perovskite CHNHPb(BrCl ) (0 ≤ x ≤ 0.19) single crystals are investigated using time-resolved photoluminescence spectroscopy with one- and two-photon femtosecond laser excitation. The introduction of chloride by substituting a fraction of the bromide leads to a decreased lattice constant compared to pure bromide perovskite ( x = 0) and a higher concentration of surface defects. The measured kinetics under one-photon excitation (1PE) shows that increasing the chloride addition quenches the photoluminescence (PL) lifetimes, due to substitution-induced surface defects. In stark contrast, upon 2PE, the PL lifetimes measured deeper in the bulk become longer with increasing chloride addition, until the halide substitution reaches the critical concentration of ∼19%. At x = 19% Cl concentration, a significant reversal of this behavior is observed indicating a change in crystal structure beyond the continuous trends observed at lower percentages of halide substitution ( x ≤ 11%). The observed opposing trends, based on 1PE versus 2PE, highlight a dichotomy between extrinsic (surface) and intrinsic (bulk) effects of chloride substitution on the carrier dynamics in lead bromide perovskites. We discuss the physical relation between halide exchange and bulk carrier lifetimes in CHNHPbBr in terms of the Rashba effect. We propose that the latter is suppressed at the surface due to disorder in the alignment of the MA and that it increases in the bulk with Cl concentration because of the reduction in lattice parameters, which compresses the space available for the MA orientational degrees of freedom.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.