Publication database
Reconfiguration of interfacial energy band structure for high-performance inverted structure perovskite solar cells
Charged defects at the surface of the organic–inorganic perovskite active layer are detrimental to solar cells due to exacerbated charge carrier recombination. Here we show that charged surface defects can be benign after passivation and further exploited for reconfiguration of interfacial energy band structure. Based on the electrostatic interaction between oppositely charged ions, Lewis-acid-featured fullerene skeleton after iodide ionization (PCBB-3N-3I) not only efficiently passivates positively charged surface defects but also assembles on top of the perovskite active layer with preferred orientation. Consequently, PCBB-3N-3I with a strong molecular electric dipole forms a dipole interlayer to reconfigure interfacial energy band structure, leading to enhanced built-in potential and charge collection. As a result, inverted structure planar heterojunction perovskite solar cells exhibit the promising power conversion efficiency of 21.1% and robust ambient stability. This work opens up a new window to boost perovskite solar cells via rational exploitation of charged defects beyond passivation.
Segregation of an amine component in a model epoxy resin at a copper interface
We have studied the chemical composition of the epoxy and amine components, HDGEBA and CBMA, of an epoxy resin in close proximity to a copper interface by using ADXPS in conjunction with SFG vibrational spectroscopy. A bilayer sample of epoxy resin and copper was first prepared on a solid substrate before etching the copper layer just before the interface with Ar+ beams. Using ADXPS, in which an incident X-ray was guided from the copper surface, it was found that the CBMA component was preferentially segregated at the copper interface, with the segregation extending over ~10 nm. SFG spectroscopy was used to confirm the above observation. Postulating that copper ions diffused from the metal copper into the internal phase during the curing process and reacted with amine groups to form copper complexes, the interfacial segregation of CBMA can be understood. This knowledge should be useful for understanding and controlling the adhesive properties of epoxy resins.
Soft x-ray emission from laser-produced strontium ions
Soft x-ray spectra, in the range from 2 nm to 9 nm, were recorded from strontium plasmas formed by pulses from 20 ps, 170 ps and 5.5 ns Nd:YAG lasers operating at the fundamental wavelength of 1064 nm. Features due to 3d–4p and 3d–4f transitions were identified by comparison with spectra from adjacent ions and atomic structure calculations with both the Cowan code and the Flexible Atomic Code. As in the spectra of ions of other elements in the fifth row of the periodic table, resonant lines 3dn–3dn−14p1, 3dn–3dn−14f1 and satellite lines 3dn−14s1–3dn−24s14p1, 3dn−14s1–3dn−24s14f1 of Δn = 1 were observed over the 3.0–8.5 nm region, emitted by 10+ to 19+ ions. These Δn = 1 transitions provide a range of narrow band emission features which may match to specific multi layer combinations for reflective optics in the extreme ultraviolet region of the spectrum.
The importance of relativistic effects on two-photon absorption spectra in metal halide perovskites
Despite intense research into the optoelectronic properties of metal halide perovskites (MHPs), sub-bandgap absorption in MHPs remains largely unexplored. Here we recorded two-photon absorption spectra of MHPs using the time-resolved microwave conductivity technique. A two-step upward trend is observed in the two-photon absorption spectrum for methylammonium lead iodide, and some analogues, which implies that the commonly used scaling law is not applicable to MHPs. This aspect is further confirmed by temperature-dependent conductivity measurements. Using an empirical multiband tight binding model, spectra for methylammonium lead iodide were calculated by integration over the entire Brillouin zone, showing compelling similarity with experimental results. We conclude that the second upward trend in the two-photon absorption spectrum originates from additional optical transitions to the heavy and light electron bands formed by the strong spin-orbit coupling. Hence, valuable insight can be obtained in the opto-electronic properties of MHPs by sub-bandgap spectroscopy, complemented by modelling.
Thermochemical writing with high spatial resolution on Ti films utilising picosecond laser
In this paper, we investigate the local oxidation of titanium thin films under the action of picosecond laser pulses. Periodical structures were recorded by the multi-beam interference scheme utilizing various numbers of laser beams, and the relationship between spatial resolution and the contrast of the structures was studied. The Raman spectra of the laser processing regions confirmed the oxidation even under the action of a single picosecond pulse. An analytical simulation of titanium film oxidation in the interference field was provided, and obtained results are correlated with the experimental data. The results of theoretical modeling show that the thermochemical effects of picosecond laser pulses allow recording periodic structures with a period of 0.65 lines per μm. The demonstrated results are important in the adaptation of technological laser systems for the manufacture of diffractive optical elements.
Third-order nonlinear optical properties of phycobiliproteins from cyanobacteria and red algae
Second hyperpolarizability (γ) measurements as well as third harmonic generation (THG) imaging was performed to determine if phycobiliproteins contribute to cyanobacteria THG, and to establish if phycobiliproteins are suitable dyes for THG microscopy. Three phycobiliproteins and one phycobilin were investigated via THG ratio γ measurements, revealing phycocyanobilin has ~7× higher γ than β-carotene, a standard THG dye. Phycobiliproteins also had large γ values, showing they are promising THG dyes. Stoichiometric summations of phycobilin γ values revealed they are the dominant source of THG signal from phycobiliproteins. THG imaging was performed to demonstrate phycobiliproteins and phycobilins can be useful THG dyes.
Vibrational Relaxation Lifetime of a Physisorbed Molecule at a Metal Surface
Previous measurements of vibrational relaxation lifetimes for molecules adsorbed at metal surfaces yielded values of 1–3 ps; however, only chemisorbed molecules have been studied. We report the first measurements of the vibrational relaxation lifetime of a molecule physisorbed to a metal surface. For CO(υ=1) adsorbed on Au(111) at 35 K the vibrational lifetime of the excited stretching mode is 49±3 ps. The long lifetime seen here is likely to be a general feature of physisorption, which involves weaker electronic coupling between the adsorbate and the solid due to bonding at larger distances.
Advanced laser scanning for highly-efficient ablation and ultrafast surface structuring: experiment and model
Ultra-short laser pulses are frequently used for material removal (ablation) in science, technology and medicine. However, the laser energy is often used inefficiently, thus, leading to low ablation rates. For the efficient ablation of a rectangular shaped cavity, the numerous process parameters such as scanning speed, distance between scanned lines, and spot size on the sample, have to be optimized. Therefore, finding the optimal set of process parameters is always a time-demanding and challenging task. Clear theoretical understanding of the influence of the process parameters on the material removal rate can improve the efficiency of laser energy utilization and enhance the ablation rate. In this work, a new model of rectangular cavity ablation is introduced. The model takes into account the decrease in ablation threshold, as well as saturation of the ablation depth with increasing number of pulses per spot. Scanning electron microscopy and the stylus profilometry were employed to characterize the ablated depth and evaluate the material removal rate. The numerical modelling showed a good agreement with the experimental results. High speed mimicking of bio-inspired functional surfaces by laser irradiation has been demonstrated.
Characterization and calibration of the Thomson scattering diagnostic suite for the C-2W field-reversed configuration experiment
The new C-2W Thomson scattering (TS) diagnostic consists of two individual subsystems for monitoring electron temperature (Te) and density (ne): one system in the central region is currently operational, and the second system is being commissioned to monitor the open field line region. Validating the performance of the TS’s custom designed system components and unique calibration of the detection system and diagnostic as a whole is crucial to obtaining high precision Te and ne profiles of C-2W’s plasma. The major components include a diode-pumped Nd:YAG laser which produces 35 pulses at up to 20 kHz, uniquely designed collection lenses with a fast numerical aperture, and uniquely designed polychromators with filters sets to optimize a Te ranging from 10 eV to 2 keV. This paper describes the design principles and techniques used to characterize the main components of the TS diagnostic on C-2W, as well as the results of Rayleigh scattering calibrations performed for the whole system response.
Charge carrier transport in polycrystalline CH3NH3PbI3 perovskite thin films in a lateral direction characterized by time-of-flight photoconductivity
We used time-of-flight photocurrent measurements to determine the role of grain boundaries in charge carrier transport in thin layers of methyl ammonium lead iodide (CH3NH3PbI3). The measurement results were compared to Kinetic Monte Carlo simulations, based on a transport model, which disentangles the transport within crystallites and hopping across grain boundaries. The observed mobilities of electrons are in the order ∼2.5 × 10−1 cm2V−1s−1. The hopping across grains is modeled with an Arrhenius-type probability rate, characterized by activation energy (Ea). It was found that the Ea estimated from the slope of a mobility-temperature dependence is in the range of ∼56–70 meV. The factors contributing to Ea are shunting pathways and the grain-size variations including energy level misalignments at the grain boundaries. These results represent a step toward a design of novel windowless organic-inorganic perovskite solar cells.