Seul-Gi Kim

The Interplay between Trap Density and Hysteresis in Planar Heterojunction Perovskite Solar Cells

Anomalous current-voltage (J-V) hysteresis in perovskite (PSK) solar cell is open to dispute, where hysteresis is argued to be due to electrode polarization, dipolar polarization, and/or native defects. However, a correlation between those factors and J-V hysteresis is hard to be directly evaluated because they usually coexist and are significantly varied depending on morphology and crystallinity of the PSK layer, selective contacts, and device architecture. In this study, without changing morphology and crystallinity of PSK layer in a planar heterojunction structure employing FA0.9Cs0.1PbI3, a correlation between J-V hysteresis and trap density is directly evaluated by means of thermally induced PbI2 regulating trap density. Increase in thermal annealing time at a given temperature of 150 °C induces growth of PbI2 on the PSK grain surface, which results in significant reduction of nonradiative recombination. Hysteresis index is reduced from 0.384 to 0.146 as the annealing time is increased from 5 to 100 min due to decrease in the amplitude of trap-mediated recombination. Reduction of hysteresis by minimizing trap density via controlling thermal annealing time leads to the stabilized PCE of 18.84% from the normal planar structured FA0.9Cs0.1PbI3 PSK solar cell.

Universal Approach toward Hysteresis-Free Perovskite Solar Cell via Defect Engineering

Organic-inorganic halide perovskite is believed to be a potential candidate for high efficiency solar cells because power conversion efficiency (PCE) was certified to be more than 22%. Nevertheless, mismatch of PCE due to current density (J)-voltage (V) hysteresis in perovskite solar cells is an obstacle to overcome. There has been much lively debate on the origin of J-V hysteresis; however, effective methodology to solve the hysteric problem has not been developed. Here we report a universal approach for hysteresis-free perovskite solar cells via defect engineering. A severe hysteresis observed from the normal mesoscopic structure employing TiO2 and spiro-MeOTAD is almost removed or does not exist upon doping the pure perovskites, CH3NH3PbI3 and HC(NH2)2PbI3, and the mixed cation/anion perovskites, FA0.85MA0.15PbI2.55Br0.45 and FA0.85MA0.1Cs0.05PbI2.7Br0.3, with potassium iodide. Substantial reductions in low-frequency capacitance and bulk trap density are measured from the KI-doped perovskite, which is indicative of trap-hysteresis correlation. A series of experiments with alkali metal iodides of LiI, NaI, KI, RbI and CsI reveals that potassium ion is the right element for hysteresis-free perovskite. Theoretical studies suggest that the atomistic origin of the hysteresis of perovskite solar cells is not the migration of iodide vacancy but results from the formation of iodide Frenkel defect. Potassium ion is able to prevent the formation of Frenkel defect since K+ energetically prefers the interstitial site. A complete removal of hysteresis is more pronounced at mixed perovskite system as compared to pure perovskites, which is explained by lower formation energy of K interstitial (-0.65 V for CH3NH3PbI3 vs -1.17 V for mixed perovskite). The developed KI doping methodology is universally adapted for hysteresis-free perovskite regardless of perovskite composition and device structure.

Effect of Cr on the high temperature oxidation of L12-type Al3Ti intermetallics

Abstract Three kinds of L1 2 -type Al 3 Ti–Cr alloys, Al 67 Ti 25 Cr 8 , Al 66 Ti 24 Cr 10 and Al 59 Ti 26 Cr 15 , were prepared by induction melting followed by thermomechanical treatment. The oxidation behavior was investigated at 1273, 1373 and 1473 K in air. The oxidation resistance of the prepared alloys was excellent, however, there were some differences for each alloy. The isothermal oxidation resistance increased in the order of Al 59 Ti 26 Cr 15 , Al 66 Ti 24 Cr 10 and Al 67 Ti 25 Cr 8 , while the order became reversed in terms of the cyclic oxidation resistance. As more Al 2 O 3 formed owing to the increased Al content in the alloy, the isothermal oxidation resistance increased, whereas the cyclic oxidation resistance decreased. The oxide scale was primarily composed of Al 2 O 3 , contaminated with Cr 2 O 3 and TiO 2 that were present mainly at the lower part the oxide scale.

High performance CNT point emitter with graphene interfacial layer

Carbon nanotubes (CNTs) have great potential in the development of high-power electron beam sources. However, for such a high-performance electronic device, the electric and thermal contact problem between the metal and CNTs must be improved. Here, we report graphene as an interfacial layer between the metal and CNTs to improve the interfacial contact. The interfacial graphene layer results in a dramatic decrease of the electrical contact resistance by an order of 2 and an increase of the interfacial thermal conductivity by 16%. Such a high improvement in the electrical and thermal interface leads to superior field emission performance with a very low turn-on field of 1.49 V μm(-1) at 10 μA cm(-2) and a threshold field of 2.00 V μm(-1) at 10 mA cm(-2), as well as the maximum current of 16 mA (current density of 2300 A cm(-2)).

Study of nanometer-thick graphite film for high-power EUVL pellicle

Extreme ultraviolet (EUV) lithography has received much attention in the semiconductor industry as a promising candidate to extend dimensional scaling beyond 10nm. Recently EUV pellicle introduction is required to improve particle level inside scanner for EUV mass production. We demonstrate that a new pellicle material, nanometer-thick graphite film (NGF), is one of the best candidates of EUV pellicle membrane. A NGF pellicle with excellent thermal (ε≥0.4 @R.T, <100nm), mechanical (415MPa @~100nm), chemical and optical (24hrs durability under exposure of EUV/H2 at 4W/cm2 with pH2~5Pa) properties can be a promising and superb candidate for EUV pellicle membrane compared to Si pellicles with capping layers.

CH3NH3PbI3 and HC(NH2)2PbI3 Powders Synthesized from Low-Grade PbI2: Single Precursor for High-Efficiency Perovskite Solar Cells

High-efficiency perovskite solar cells are generally fabricated by using highly pure (>99.99 %) PbI2 mixed with an organic iodide in polar aprotic solvents. However, the use of such an expensive chemical may impede progress toward large-scale industrial applications. Here, we report on the synthesis of perovskite powders by using inexpensive low-grade (99 %) PbI2 and on the photovoltaic performance of perovskite solar cells prepared from a powder-based single precursor. Pure APbI3 [A=methylammonium (MA) or formamidinium (FA)] perovskite powders were synthesized by treating low-grade PbI2 with MAI or FAI in acetonitrile at ambient temperature. The structural phase purity was confirmed by X-ray diffraction. The solar cell with a MAPbI3 film prepared from the synthesized perovskite powder demonstrated a power conversion efficiency (PCE) of 17.14 %, which is higher than the PCE of MAPbI3 films prepared by using both MAI and PbI2 as precursors (PCE=13.09 % for 99 % pure PbI2 and PCE=16.39 % for 99.9985 % pure PbI2 ). The synthesized powder showed better absorption and photoluminescence, which were responsible for the better photovoltaic performance. For the FAPbI3 powder, a solution with a yellow non-perovskite δ-FAPbI3 powder synthesized at room temperature was found to lead to a black perovskite film, whereas a solution with the black perovskite α-FAPbI3 powder synthesized at 150 °C was not transformed into a black perovskite film. The α↔δ transition between the powder and film was assumed to correlate with the difference in the iodoplumbates in the powder-dissolved solution. An average PCE of 17.21 % along with a smaller hysteresis [ΔPCE=PCEreverse -PCEforward )=1.53 %] was demonstrated from the perovskite solar cell prepared by using δ-FAPbI3 powder; this PCE is higher than the average PCE of 17.05 % with a larger hysteresis (ΔPCE=2.71 %) for a device based on a conventional precursor solution dissolving MAI with high-purity PbI2 . The smaller hysteresis was indicative of fewer defects in the resulting FAPbI3 film prepared by using the δ-FAPbI3 powder.

FA0.88Cs0.12PbI3−x(PF6)x Interlayer Formed by Ion Exchange Reaction between Perovskite and Hole Transporting Layer for Improving Photovoltaic Performance and Stability

Interface engineering to form an interlayer via ion exchange reaction is reported. A FA0.88 Cs0.12 PbI3 formamidinium (FA) perovskite layer is first prepared, then FAPF6 solution with different concentrations is spin-coated on top of the perovskite film, which leads to a partial substitution of iodide by PF6- ion. The second phase with nominal composition of FA0.88 Cs0.12 PbI3-x (PF6 )x is grown at the grain boundary, which has island morphology and its size depends on the FAPF6 solution concentration. The lattice is expanded and bandgap is reduced due to inclusion of larger PF6- ions. The power conversion efficiency (PCE) is significantly enhanced from 17.8% to 19.3% as a consequence of improved fill factor and open-circuit voltage (Voc ). In addition, current-voltage hysteresis is reduced. Post-treatment with FAPF6 reduces defect density and enhances carrier lifetime, which is responsible for the improved photovoltaic performance and reduced hysteresis. The unencapsulated device with post-treated perovskite film demonstrates better stability than the pristine perovskite, where the initial PCE retains over 80% after 528 h exposure under relative humidity of around 50-70% in the dark and 92% after 360 h under one sun illumination.

Rear-Surface Passivation by Melaminium Iodide Additive for Stable and Hysteresis-less Perovskite Solar Cells

Surface passivation of perovskite grains is one of the promising methods to reduce recombination and improve stability of perovskite solar cells (PSCs). We herein report the effect of a melaminium iodide additive on the photovoltaic performance of PSCs based on (FAPbI3)0.875(CsPbBr3)0.125 perovskite. Cyclic -C═N- and primary amine in melamine are a good hydrogen bond acceptor and Lewis base, which can interact with both the organic cation and Lewis acidic lead iodide in the perovskite film. Melaminium iodide is synthesized and added to the precursor solution, which is directly spin-coated to form the perovskite film. The presence of melaminium iodide additive reduces the trap density from 1.02 × 1016 to 0.645 × 1016 cm-3, which leads to the reduction of nonradiative recombination and thereby improving the mean open-circuit voltage and the fill factor from 1.054 to 1.095 V and from 0.693 to 0.725 V, receptively. In addition, photocurrent-voltage hysteresis is reduced by the melaminium iodide additive, which results in an enhanced average power conversion efficiency, obtained from reverse and forward scanned data, from 15.86 to 17.32%. Time-resolved photoluminescence confirms that melaminium iodide plays a more important role in passivating the rear surface of the perovskite layer contacting the hole transporting spiro-MeOTAD layer. An aging test under a relative humidity of 65% reveals that melaminium iodide improves stability because of the suppression of the defect evolved by moisture.