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Volatile A-cation halide (AX) additives such as formamidinium chloride and methylammonium chloride have been widely employed for high-efficiency perovskite solar cells (PSCs). However, it remains unstudied how they influence the perovskite film stoichiometry and the solar cell performance and operational stability. Hereby, our work shows that over annealing of formamidinium chloride-containing perovskite films leads to a Pb-rich surface, resulting in a high initial efficiency, which however decays during maximum power point tracking (MPPT). On the contrary, perovskite films obtained by a shorter annealing time at the same temperature provide good stability during MPPT but a lower initial efficiency. Thus, we deduce that an optimal annealing is vital for both high efficiency and operational stability, which is then confirmed in the case where methylammonium chloride additive is used. With optimized perovskite annealing conditions, we demonstrate efficient and stable p-i-n PSCs that show a best power conversion efficiency of 20.7% and remain 90% of the initial performance after a 200 h MPPT at 60 °C under simulated 1 sun illumination with high UV content. Our work presents a comprehensive understanding on how volatile AX impacts perovskite film stoichiometry and its correlation to the device performance and operational stability, providing a new guideline for fabricating high-efficiency and operationally stable PSCs.

Volatile A-cation halide (AX) additives such as formamidinium chloride and methylammonium chloride have been widely employed for high-efficiency perovskite solar cells (PSCs). However, it remains unstudied how they influence the perovskite film stoichiometry and the solar cell performance and operational stability. Hereby, our work shows that over annealing of formamidinium chloride-containing perovskite films leads to a Pb-rich surface, resulting in a high initial efficiency, which however decays during maximum power point tracking (MPPT). On the contrary, perovskite films obtained by a shorter annealing time at the same temperature provide good stability during MPPT but a lower initial efficiency. Thus, we deduce that an optimal annealing is vital for both high efficiency and operational stability, which is then confirmed in the case where methylammonium chloride additive is used. With optimized perovskite annealing conditions, we demonstrate efficient and stable p–i–n PSCs that show a best power conversion efficiency of 20.7% and remain 90% of the initial performance after a 200 h MPPT at 60 °C under simulated 1 sun illumination with high UV content. Our work presents a comprehensive understanding on how volatile AX impacts perovskite film stoichiometry and its correlation to the device performance and operational stability, providing a new guideline for fabricating high-efficiency and operationally stable PSCs.

Gallium nitride (GaN) grown on Si by metalorganic chemical vapor deposition was analyzed using high-resolution, high-energy x-ray photoelectron spectroscopy (HAXPES). The HAXPES spectra of GaN obtained using monochromatic Cr Kα radiation at 5414.7 eV include a survey scan (Al Kα) and high-resolution spectra of Ga 3d, Ga 2p3/2, Ga 3p, Ga LMM, N 1s, C 1s, and O 1s.

For porous low-k film to be integrated into the next generation of interconnects, the pores need to be sealed against metal ions and barrier precursors. Self-assembled monolayers (SAMs) from organosilane precursor are spin coated onto 300mmk=2.2 low-k wafers. Two solvents, propylene glycol monomethyl ether acetate (PGMEA) and methanol with different dielectric constant of 8.3 and 20.1, are evaluated in terms of SAMs layer quality and sealing efficiency at coupon level. SAMs deposited from PGMEA show better sealing than SAMs deposited from methanol and therefore are selected for upscaling. Full wafer spin coating results show that a concentration of 0.05mM or below results in a partial coverage and a tilt angle as high as 70° from the backbone to the normal. Aggregation is observed for all tested concentrations and is worse for higher concentrations, which is possibly induced by the non-negligible presence of water in PGMEA solvents. In order to test the sealing efficiency of the SAMs layer against metal barrier precursors, MnN films by chemical vapor deposition (CVD) and TaNx/Ta (TNT) films by physical vapor deposition (PVD) are deposited on SAM coated low-k wafers. HfO2 is also deposited by Atomic layer deposition (ALD), which is not considered as a barrier but to test the sealing against ALD precursors. Depth profiling Rutherford Backscattering Spectrometry (RBS) measurements indicate an effective sealing of SAMs against CVD and ALD precursors but not against PVD barrier. Display Omitted SAMs are spin coated onto 300mm low-k wafers. After SAMs deposition, źk is 0.1 and decreases to 0.03 after annealing.Solvent dielectric constant affect the pre-condensation of SAMs and therefore sealing.RBS measurements shows that SAMs seal against MnN by CVD but not TNT by PVD.

The products of the solid state reaction involving ultra-thin Ni film (6nm) and Si1-xGex layers (Ge 25 and 55at.%), were analysed using sheet resistance (Rs), glancing angle X-ray diffraction (GIXRD), scanning electron and atomic force microscopy (SEM, AFM) techniques. The reaction was carried out via rapid thermal process (RTP) annealing using two different steps (RTP1 and RTP2) while applying a selective etch (SE) in between them. The intermediate and the end reaction products resulting after RTP1 and RTP2 were found to be dependent on the Ge content, forming Ni-rich silicide (Ni2Si) and NiSi on Si75Ge25, while Ni-rich germanide (Ni5Ge3) and NiGe were obtained by using Si45Ge55. Though the onset of intermediate Ni-rich silicide or germanide phase formation occurs at similar RTP1 temperature (275?C), the reaction completion to yield low resistive phase NiSi or NiGe phase results at different RTP2 temperatures (400?C vs 350?C). Based on the volume expansion, a resistivity value of 25µ?cm was obtained for the synthesized NiGe (12nm) and NiSi (14nm) layers. Independent of the phases obtained, the films were found to be closed and homogeneous and exhibit rms roughness of 0.5-0.8nm as evidenced by SEM and AFM analysis. Thermal stability studies carried out on NiSi and NiGe thin films, post RTP1/RTP2, show the latter phase to have limited stability and result in Rs degradation starting already at 475?C due to phase decomposition. Display Omitted The reaction of ultrathin Ni film with Si1-xGex layer (x: 25 and 55at.%) is studied.Depending of Ge%, NiSi or NiGe is obtained but with different formation temperatures.The morphology, roughness and resistivity were found to be the same for NiSi and NiGe.NiGe on Si45Ge55 has limited thermal stability compared to NiSi on Si75Ge25.

The atomic layer deposition (ALD) of Ta2O5 and TaSiOx from TaCl5, SiCl4, and H2O is reported. Both processes are influenced by the concomitant etching of Ta2O5 and TaSiOx by TaCl5. The optimum deposition temperature is found to be 250 °C for both Ta2O5 and TaSiOx. For lower deposition temperatures, the large Cl contamination leads to poor dielectric properties of the films, whereas higher temperatures lead to poor within-wafer (WiW) thickness non-uniformity due to etching. Si incorporation is limited to Si/(Si + Ta) ∼ 0.65 because of the slow adsorption kinetics of SiCl4 on SiOH-terminated surfaces. Under optimum conditions, amorphous films with good dielectric quality are obtained.

A low-temperature (225-300 °C) solid-vapor reaction process is reported for the synthesis of ultrathin NiGe films (∼6-23 nm) on 300 mm Si wafers covered with thermal oxide. The films were prepared via catalytic chemical vapor reaction of germane (GeH4) gas with physical vapor deposited (PVD) Ni films of different thickness (2-10 nm). The process optimization by investigating GeH4 partial pressure, reaction temperature, and time shows that low resistive, stoichiometric, and phase pure NiGe films can be formed within a broad window. NiGe films crystallized in an orthorhombic structure and were found to exhibit a smooth morphology with homogeneous composition as evidenced by glancing angle X-ray diffraction (GIXRD), scanning electron microscopy (SEM), atomic force microscopy (AFM), and Rutherford back-scattering (RBS) analysis. Transmission electron microscopy (TEM) analysis shows that the NiGe layers exhibit a good adhesion without voids and a sharp interface on the thermal oxide. The NiGe films were found to be morphologically and structurally stable up to 500 °C and exhibit a resistivity value of 29 μΩ cm for 10 nm NiGe films.

We report on aggressively scaled replacement metal gate, high-k last (RMG-HKL) planar and multi-gate fin field-effect transistor (FinFET) devices, systematically investigating the impact of post high-k deposition thermal (PDA) and plasma (SF6) treatments on device characteristics, and providing a deeper insight into underlying degradation mechanisms. We demonstrate that: 1) substantially reduced gate leakage (J G) and noise can be obtained for both type of devices with PDA and F incorporation in the gate stack by SF6, without equivalent oxide thickness (EOT) penalty; 2) SF6 enables improved mobility and reduced interface trapped charge density (N it) down to narrower fin devices [fin width (W Fin) ≥ 5 nm], mitigating the impact of fin patterning and fin sidewall crystal orientations, while allowing a simplified dual-effective work function (EWF) CMOS scheme suitable for both device architectures; 3) PDA yields smaller, in absolute values, PMOS threshold voltage |V T|, and substantially improved reliability behavior due to reduction of bulk defects.