Thomas Jaouen

A Ga-doped SnO2 mesoporous contact for UV stable highly efficient perovskite solar cells

Increasing the stability of perovskite solar cells is a major challenge for commercialization. The highest efficiencies so far have been achieved in perovskite solar cells employing mesoporous TiO2 (m-TiO2). One of the major causes of performance loss in these m-TiO2-based perovskite solar cells is induced by UV-radiation. This UV instability can be solved by replacing TiO2 with SnO2; thus developing a mesoporous SnO2 (m-SnO2) perovskite solar cell is a promising approach to maximise efficiency and stability. However, the performance of mesoporous SnO2 (m-SnO2) perovskite solar cells has so far not been able to rival the performance of TiO2 based perovskite solar cells. In this study, for the first time, high-efficiency m-SnO2 perovskite solar cells are fabricated, by doping SnO2 with gallium, yielding devices that can compete with TiO2 based devices in terms of performance. We found that gallium doping severely decreases the trap state density in SnO2, leading to a lower recombination rate. This, in turn, leads to an increased open circuit potential and fill factor, yielding a stabilised power conversion efficiency of 16.4%. The importance of high-efficiency m-SnO2 based perovskite solar cells is underlined by stability data, showing a marked increase in stability under full solar spectrum illumination.

Layer-resolved study of Mg atom incorporation at the MgO/Ag(001) buried interface.

By combining x-ray excited Auger electron diffraction experiments and multiple scattering calculations we reveal a layer-resolved shift for the Mg KL23L23 Auger transition in MgO ultrathin films (4-6 Å) on Ag(001). This resolution is exploited to demonstrate the possibility of controlling Mg atom incorporation at the MgO/Ag(001) interface by exposing the MgO films to a Mg flux. A substantial reduction of the MgO/Ag(001) work function is observed during the exposition phase and reflects both band-offset variations at the interface and band bending effects in the oxide film.

Short-range phase coherence and origin of the 1T-TiSe2 charge density wave

The impact of variable Ti self-doping on the 1T−TiSe2 charge density wave (CDW) is studied by scanning tunneling microscopy. Supported by density functional theory, we show that agglomeration of intercalated-Ti atoms acts as preferential nucleation centers for the CDW that breaks up in phase-shifted CDW domains whose size directly depends on the intercalated-Ti concentration and which are separated by atomically sharp phase boundaries. The close relationship between the diminution of the CDW domain size and the disappearance of the anomalous peak in the temperature-dependent resistivity allows to draw a coherent picture of the 1T−TiSe2 CDW phase transition and its relation to excitons.

Tuning the Schottky barrier height at MgO/metal interface

We present an experimental investigation of the interface electronic structure of thin MgO films epitaxially grown on Ag(001) by x-ray and ultraviolet photoemission spectroscopy as a function of the oxide growth conditions. It is shown that the Schottky barrier height at MgO/metal interface can be tuned over 0.7 eV by a modification of the oxygen partial pressure or the sample temperature. These experimental results are explained in the framework of the extended Schottky-Mott model and the MgO-induced polarization effect by Mg enrichment of the silver surface region.

Induced work function changes at Mg-doped MgO/Ag(001) interfaces: Combined Auger electron diffraction and density functional study

The properties of MgO/Ag(001) ultrathin films with substitutional Mg atoms in the interface metal layer have been investigated by means of Auger electron diffraction experiments, ultravio-let photoemission spectroscopy, and density functional theory (DFT) calculations. Exploiting the layer-by-layer resolution of the Mg KL23L23 Auger spectra and using multiple scattering calcula-tions we first determine the inter-layer distances as well as the morphological parameters of the MgO/Ag(001) system with and without Mg atoms incorporated at the interface. We find that the Mg atom incorporation drives a strong distortion of the interface layers and that its impact on the metal/oxide electronic structure is an important reduction of the work function (0.5 eV) related to band-offset variations at the interface. These experimental observations are in very good agreement with our DFT calculations which reproduce the induced lattice distortion and which reveal (through a Bader analysis) that the increase of the interface Mg concentration results in an electron transfer from Mg to Ag atoms of the metallic interface layer. Although the local lattice distortion appears as a consequence of the attractive (repulsive) Coulomb interaction between O 2− ions of the MgO interface layer and the nearest positively (negatively) charged Mg (Ag) neighbors of the metallic interface layer, its effect on the work function reduction is only limited. Finally, an analysis of the induced work function changes in terms of charge transfer, rumpling, and electrostatic compression contributions is attempted and reveals that the metal/oxide work function changes induced by inter-face Mg atoms incorporation are essentially driven by the increase of the electrostatic compression effect.

Excited states at interfaces of a metal-supported ultrathin oxide film

We report layer-resolved measurements of the \textit{unoccupied} electronic structure of ultrathin MgO films grown on Ag(001). The metal-induced gap states at the metal/oxide interface, the oxide band gap as well as a surface core exciton involving an image-potential state of the vacuum are revealed through resonant Auger spectroscopy of the Mg

Local resilience of the 1T-TiSe2 charge density wave to Ti self-doping

KL_{23}L_{23}

Layer-Resolved Photoemission Study of Doped Ag-Supported Ultrathin MgO Films

Auger transition. Our results demonstrate how to obtain new insights on \textit{empty} states at interfaces of metal-supported ultrathin oxide films.

Selective Probing of Hidden Spin-Polarized States in Inversion-Symmetric Bulk MoS2

In Ti-intercalated self-doped 1T-TiSe2 crystals, the charge density wave (CDW) superstructure induces two nonequivalent sites for Ti dopants. Recently, it has been shown that increasing Ti doping dramatically influences the CDW by breaking it into phase-shifted domains. Here, we report scanning tunneling microscopy and spectroscopy experiments that reveal a dopant-site dependence of the CDW gap. Supported by density functional theory, we demonstrate that the loss of the long-range phase coherence introduces an imbalance in the intercalated-Ti site distribution and restrains the CDW gap closure. This local resilient behavior of the 1T-TiSe2 CDW reveals an entangled mechanism between CDW, periodic lattice distortion, and induced nonequivalent defects.

Three-dimensional momentum-resolved electronic structure of 1T-TiSe2: A combined soft-x-ray photoemission and density functional theory study

MgO/Ag(001) ultrathin films doped with interfacial Mg atoms are studied with layer-resolved Auger electron diffraction experiments, ultraviolet photoemission measurements, multiple scattering calculations, and density functional theory (DFT) calculations. The Mg atom intercalation at the MgO/Ag(001) interface induces a strong rumpling of the interface layers as well as a lowering of the work function related to interface electronic structure changes. DFT analysis of the metal-oxide interactions responsible for the interface dipole reproduces the experimental observations and reveals that the metal/oxide work function changes essentially originate in an increased electrostatic compression effect.