Inorganic-organic interfaces are important for enhancing the power conversion efficiency of silicon-based solar cells through singlet exciton fission (SF). We elucidated the structure of the first monolayers of tetracene (Tc), a SF molecule, on hydrogen-passivated Si(111) [H-Si(111)] and hydrogenated amorphous Si (a-Si:H) by combining near-edge X-ray absorption fine structure (NEXAFS) and X-ray photoelectron spectroscopy (XPS) experiments with density functional theory (DFT) calculations. For samples grown at or below substrate temperatures of 265 K, the resulting ultrathin Tc films are dominated by almost upright-standing molecules. The molecular arrangement is very similar to the Tc bulk phase, with only slightly higher average angle between the conjugated molecular plane normal and the surface normal ($α$) around 77°. Judging from carbon K-edge X-ray absorption spectra, the orientation of the Tc molecules are almost identical when grown on H-Si(111) and a-Si:H substrates as well as for (sub)mono- to several-monolayer coverages. Annealing to room temperature, however, changes the film structure towards a smaller $α$ of about 63°. A detailed DFT-assisted analysis suggests that this structural transition is correlated with a lower packing density and requires a well-chosen amount of thermal energy. Therefore, we attribute the resulting structure to a distinct monolayer configuration that features less inclined, but still well-ordered molecules. The larger overlap with the substrate wavefunctions makes this arrangement attractive for an optimized interfacial electron transfer in SF-assisted silicon solar cells.
Singlet fission in tetracene generates two triplet excitons per absorbed photon. If these triplet excitons can be effectively transferred into silicon (Si) then additional photocurrent can be generated from photons above the bandgap of Si. This could alleviate the thermalization loss and increase the efficiency of conventional Si solar cells. Here we show that a change in the polymorphism of tetracene deposited on Si due to air exposure, facilitates triplet transfer from tetracene into Si. Magnetic field-dependent photocurrent measurements confirm that triplet excitons contribute to the photoc…
Time-resolved two color pump-probe polarization spectroscopy was performed at room temperature on SrTiO3 films grown directly on Si with film thickness varying from 2 nm to 7.8 nm. The E soft mode with a characteristic frequency of 0.2 THz is impulsively generated and measured in these coherently strained tetragonal phase SrTiO3 thin films. Another over-damped signal observed indicates the possible relaxational hopping of Ti ion between double potential wells. The dependence of the coherent phonon signal on pump and probe laser polarization helps to identify the phonon modes.
Ultrathin InAs nanowires (NW) with one-dimensional (1D) sub-band structure are promising materials for advanced quantum-electronic devices, where dimensions in the sub-30 nm diameter limit together with post-CMOS integration scenarios on Si are much desired. Here, we demonstrate two site-selective synthesis methods that achieve epitaxial, high aspect ratio InAs NWs on Si with ultrathin diameters below 20 nm. The first approach exploits direct vapor-solid growth to tune the NW diameter by interwire spacing, mask opening size and growth time. The second scheme explores a unique reverse-reaction …
Anisotropic phonon transport along different lattice directions of two-dimensional (2D) materials has been observed, however, the effect decreases with increasing the thickness beyond a few atomic layers. Here we establish a novel mechanism to induce anisotropic phonon transport in quasi-2D materials with isotropic symmetry. The phonon propagation is guided by resonance hybridization with surface nanostructures. We demonstrate that the thermal conductivity of 3 nm-thick silicon membrane with surface nanofins is greater by $\sim50\%$ parallel to the fins than that perpendicular to the fins.
Investigation of the spin Hall effect in gold has triggered increasing interest over the past decade, since gold combines the properties of a large bulk spin diffusion length and strong interfacial spin-orbit coupling. However, discrepancies between the values of the spin Hall angle of gold reported in the literature have brought into question the microscopic origin of the spin Hall effect in Au. Here, we investigate the thickness dependence of the spin-charge conversion efficiency in single Au films and ultrathin Au/Si multilayers by non-local transport and spin-torque ferromagnetic resonance…
Atomic layer deposition (ALD) is a key technique for the continued scaling of semiconductor devices, which increasingly relies on reproducible and scalable processes for interface manipulation of 3D structured surfaces on the atomic scale. While ALD allows the synthesis of conformal films at low temperature with utmost control over the thickness, atomically-defined closed coatings and surface modifications are still extremely difficult to achieve because of three-dimensional growth during nucleation. Here, we present a route towards sub-nanometer thin and continuous aluminum oxide (AlOx) coati…
Interface effects and dielectric mismatch in ultrathin silicon on insulator films
CNR-IMM（意大利国家研究委员会材料研究所）；Università degli Studi di Milano-Bicocca（米兰比可卡大学）；Institut für Experimentelle Physik, TU Bergakademie Freiberg（弗莱贝格矿业科技大学实验物理研究所）；Università del Piemonte Orientale ‘‘A. Avogadro’’（皮埃蒙特东方大学）；Institut für Angewandte Physik, TU Bergakademie Freiberg（弗莱贝格矿业科技大学应用物理研究所）；University of Torino（都灵大学）
Ultrathin cerium oxide films have been deposited on chlorine, gallium, and silver passivated Si(111) by reactive molecular beam epitaxy in a comparative study. The crystallinity of these films has been characterized by x-ray standing waves while the oxidation state of the rare-earth oxide (REOx) films and the chemical interface composition have been revealed by hard x-ray photoelectron spectroscopy. The use of Cl as passivating agent results in the epitaxial growth of highly crystalline REOx films with the RE metal in the 3+ oxidation state while effectively suppressing silicate and silicon ox…
Time-resolved study of carbonization and growth of ultrathin 3C-SiC on Si(111) under ultra-high vacuum
Central European Institute of Technology, Brno University of Technology（中欧技术研究所，布尔诺理工大学）；Institute of Physical Engineering, Brno University of Technology（物理工程学院，布尔诺理工大学）
Silicon inverted pyramids arrays have been suggested as one of the most promising structure for high-efficient ultrathin solar cells due to their ability of superior light absorption and low enhancement of surface area. However, the existing techniques for such fabrication are either expensive or not able to create appropriate structure. Here, we present a lithography free method for the fabrication of inverted pyramid arrays by using a modified metal assisted chemical etching (MACE) method. The size and inter-inverted pyramids spacing can also be controlled through this method. We used an iso…
Density of the polyacrylamide ultrathin films has been studied using X-ray reflectivity technique. Two sources (one powder and another aqueous solution) of polyacrylamide were used to prepare spin coated films on silicon substrate. Light scattering measurements show that the polymer chains were unentangled in a concentrated (4 mg/ml) as well as in a dilute (2 mg/ml) solution prepared from the powder, whereas the solution (4 mg/ml) prepared by diluting the solution source shows entangled chain morphology. Three sets of films of different thicknesses were prepared using the three solutions by sp…
In recent years, thin-film organic field-effect transistors (OFETs) have begun to be considered as a possible alternative to the hydrogenated amorphous silicon thin-film transistors (a-Si:H TFT's) used in active matrix flat panel displays and other large-area electronics applications. Low-temperature processability, low-cost fabrication and compatibility with arbitrary substrates are some of the promising advantages of OFETs, among others. Of the many organic materials available, pentacene, in particular, is one of the leading candidates for use in current thin-film OFET architectures - this b…
Despite the youthfulness of hybrid halide perovskite solar cells, their efficiencies are currently comparable to commercial silicon and have surpassed quantum-dots solar cells. Yet, the scalability of these devices is a challenge due to their low reproducibility and stability under environmental conditions. However, the methods reported to date to tackle such issues recurrently involve the use of solvent methods that would further complicate their transfer to industry. Herein we present a reliable alternative relaying in the implementation of an ultrathin plasma polymer as passivation interfac…
One way for solar cell efficiencies to overcome the Shockley-Queisser limit is downconversion of high-energy photons using singlet fission (SF) in polyacenes like tetracene (Tc). SF enables generation of multiple excitons from the high-energy photons which can be harvested in combination with Si. In this work we investigate the use of lead sulfide quantum dots (PbS QDs) with a band gap close to Si as an interlayer that allows Foerster Resonant Energy Transfer (FRET) from Tc to Si, a process that would be spin-forbidden without the intermediate QD step. We investigate how the conventional FRET …
Thin films of transition metal oxides open up a gateway to nanoscale electronic devices beyond silicon characterized by novel electronic functionalities. While such films are commonly prepared in an oxygen atmosphere, they are typically considered to be ideally terminated with the stoichiometric composition. Using the prototypical correlated metal SrVO$_3$ as an example, it is demonstrated that this idealized description overlooks an essential ingredient: oxygen adsorbing at the surface apical sites. The oxygen adatoms, which persist even in an ultrahigh vacuum environment, are shown to severe…
The effect of annealing on the dynamical behavior of swelling for ultrathin polyacrylamide films deposited on silicon substrates have been studied using X-ray reflectivity technique. The spin coated polyacrylamide films of similar thicknesses were annealed at various temperatures below and above the glass transition temperature of the polymer. The electron density of the films was found to increase systematically on annealing. The swelling dynamics of the annealed films were found to have systematic dependence on the temperature of annealing. The interaction between the substrate and the polym…
Recently high density (HD) nonmagnetic (NM) cobalt has been discovered in a cobalt thin film, grown on Si(111). This cobalt film had a natural cobalt oxide at the top. The oxide layer forms when the film is taken out of the electron-beam deposition chamber and exposed to air. Thin HD NM cobalt layers were found near the cobalt/silicon and the cobalt-oxide/cobalt interfaces, while the thicker mid-depth region of the film was hcp cobalt with normal density and normal magnetic moment. If an ultrathin film of gold is grown on the cobalt layer, before exposing it to air, the oxidation of the cobalt…
Silicene is one of the most promising 2D materials for the realization of next-generation electronic devices, owing to its high carrier mobility and bandgap tunability through the imposition of an external electric field. To exploit this fundamental characteristic, it is necessary to engineer an insulating layer that can be interfaced directly to silicene without perturbing its bidimensional nature. At the same time, this insulating layer should exhibit low leakage currents even when highly scaled, to fully exploit the advantages of using a 2D material at the core of the device. CaF$_2$ is kno…
Electric gating can strongly modulate a wide variety of physical properties in semiconductors and insulators, such as significant changes of conductivity in silicon, appearance of superconductivity in SrTiO3, the paramagnet-ferromagnet transition in (In,Mn)As and so on. The key to such modulation is charge accumulation in solids. Thus, it has been believed that such modulation is out of reach for conventional metals where the number of carriers is too large. However, success in tuning the Curie temperature of ultrathin cobalt gave hope of finally achieving such degree of control even in metall…
The long theorized two-dimensional allotrope of SiC has remained elusive amid the exploration of graphenelike honeycomb structured monolayers. It is anticipated to possess a large direct band gap (2.5 eV), ambient stability, and chemical versatility. While $sp^{2}$ bonding between silicon and carbon is energetically favorable, only disordered nanoflakes have been reported to date. Here we demonstrate large-area, bottom-up synthesis of monocrystalline, epitaxial monolayer honeycomb SiC atop ultrathin transition metal carbide films on SiC substrates. We find the 2D phase of SiC to be almost plan…
An application of the radiolysis method using X-ray synchrotron beam is developed as a novel approach to the synthesis of metal-organic films with controlled shapes and thickness. We demonstrate that a Langmuir monolayer deposited onto a silver ion-containing subphase, irradiated by an incident beam impinging below the critical angle for total reflection, induces the synthesis of a stable nanostructured silver-organic ultrathin film at the air-water interface. The X-ray scattering is also used to monitor in situ the structure of the silver layer during the synthesis process. The layer is obser…
Two-dimensional (2D) materials van der Waals heterostructures (vdWHs) provides a revolutionary route towards high-performance solar energy conversion devices beyond the conventional silicon-based pn junction solar cells. Despite tremendous research progress accomplished in recent years, the searches of vdWHs with exceptional excitonic solar cell conversion efficiency and optical properties remain an open theoretical and experimental quest. Here we show that the vdWH family composed of MoSi$_2$N$_4$ and WSi$_2$N$_4$ monolayers provides a compelling material platform for developing high-performa…
Perovskite semiconductors have demonstrated outstanding external luminescence quantum yields, enabling high power conversion efficiencies (PCE). However, the precise conditions to advance to an efficiency regime above monocrystalline silicon cells are not well understood. Here, we establish a simulation model that well describes efficient p-i-n type perovskite solar cells and a range of different experiments. We then study important device and material parameters and we find that an efficiency regime of 30% can be unlocked by optimizing the built-in potential across the perovskite layer by usi…
