Light-induced charge transfer at the CH3NH3PbI3/TiO2 interface-a low-temperature photo-electron paramagnetic resonance assay

Pavao Roko Andricevic, Philippe Bugnon, László Forró, Anastasiia Glushkova, Endre Horvath, Márton Kollár, Konstantins Mantulnikovs, Bálint Náfrádi, Lidia Rossi, Andrzej Sienkiewicz, Péter Szirmai
IOP PUBLISHING LTD, 2020
Article

Résumé

The performance of organic-inorganic metal halide perovskites-based (MHPs) photovoltaic devices critically depends on the design and material properties of the interface between the light-harvesting MHP layer and the electron transport layer (ETL). Therefore, the detailed insight into the transfer mechanisms of photogenerated carriers at the ETL/MHP interface is of utmost importance. Owing to its high charge mobilities and well-matched band structure with MHPs, titanium dioxide (TiO2) has emerged as the most widely used ETL material in MHPs-based photovoltaic devices. Here, we report a contactless method to directly track the photo-carriers at the ETL/MHP interface using the technique of low-temperature electron paramagnetic resonance (EPR) in combination with in situ illuminations (Photo-EPR). Specifically, we focus on a model nanohybrid material consisting of TiO2-based nanowires (TiO(2)NWs) dispersed in the polycrystalline methylammonium lead triiodide (MAPbI(3)) matrix. Our approach is based on observation of the light-induced decrease in intensity of the EPR signal of paramagnetic Ti3+ ( S = 1 / 2 ) in non-stoichiometric TiO(2)NWs. We associate the diminishment of the EPR signal with the photo-excited electrons that cross the ETL/MHP interface and contribute to the conversion of Ti3+ states to EPR-silent Ti2+ states. Overall, we infer that the technique of low-temperature Photo-EPR is an effective strategy to study the transfer mechanisms of photogenerated carriers at the ETL/MHP interface in MAPbI(3)-based photovoltaic and photoelectronic systems.

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https://infoscience.epfl.ch/record/281894?ln=fr

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Investigation of interactions in two-dimensional electron gases with angular resolved photoemission spectroscopy

Carola Strasser

In this thesis, angular resolved photoemission spectroscopy (ARPES) is used to study the electronic structure of different two-dimensional electron systems (2DES). This technique is very surface sensitive and the most direct method to probe the surface band structure of a system. In addition to the band dispersion also signatures from interactions can be detected with ARPES. A careful analysis of peak position and linewidth gives access to the complex self-energy Sigma, which describes the energy renormalization and the lifetime of the electrons due to many-body interactions. By using circularly polarized light it is possible to excite electrons selectively and to extract additional information about the electronic states in the surface. 2DESs exist typically either at interfaces or at surfaces. We put our focus on the surface states of topological insulators and investigate Bi2Te2Se and TiTe1.5Se0.5. The first is known to be a topological insulator with the Fermi energy located in the bulk band gap. A time-dependent doping behavior is observed and we show that the Coulomb interaction in this material is strongly dependent on the charge carrier density and not negligible for very low concentrations. TiTe1.5Se0.5 was predicted to be a topological insulator. We are able to present the surface band structure, but due to the fact that ARPES can only probe the occupied states it is impossible to see the predicted topological surface states. The third system under investigation is a monolayer of epitaxial graphene on SiC(0001) decorated by small amounts of Tl adatoms. ARPES measurements at very low temperature and very low impurity concentrations show that Tl adatoms not only give rise to electron doping but have also a large effect on the quasiparticle scattering rate. The adatoms introduce disorder and act on the graphene electronic structure both as Coulomb long-range scatterers as well as short-range scatterers with a delta-like potential. We show that also for charged impurities short-range scattering can play an important role and is not always negligible. By modeling the self-energy for long- and short-range scattering, we are able to extract a strong short-range scattering potential delta=-3.2 +/- 1 eV. A detailed understanding of the underlying scattering mechanisms in graphene is very important for the development of novel impurity-graphene-based electronics. ARPES experiments are also performed on the surface alloys on Ag(111). For these measurements, we use circularly polarized light and take advantage of the fact that the interaction between light and matter changes for different polarizations. Surface alloys on Ag(111) are formed by depositing 1/3 of a monolayer of bismuth or antimony on the clean Ag(111) surface, where every third Ag atom is replaced by such an alloy atom. These systems are known for their Rashba type spin splitting and the resulting chiral spin structure in the two-dimensional (2D) band structure. We show that circular dichroism (CD) in the angular distribution of the photoelectrons depends strongly on the experimental setup and the energy of the photons. Only under special circumstances it is possible to use CD to access the orbital angular momentum and - in systems with high spin-orbit coupling - maybe even the spin texture of the surface. Because of the final state effects, interpretation of CD data is quite complicated and has to be done very cautiously.

EPFL2015

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Developing a high-performance catalyst and establishing a catalytic mechanism for understanding the catalytic activity are crucial to new generation photovoltaic technology. In this work, we present a feasible and general route to synthesize a bio-based porous carbon (BPC) supported ZnNb2O6 hybrid catalyst with a unique network structure, providing an effective means for electron transport between the electrode and the external circuit. Benefitting from the synergistic effect of ZnNb2O6 and BPC, a photovoltaic device assembled with the nanohybrid yields a power conversion efficiency of 8.83%, which is superior to that of pristine ZnNb2O6-based and conventional Pt-based cells (7.15% and 7.14%). Systematic electrochemical evaluations of the hybrid catalysts exhibit promising stability for practical application in photovoltaics. Contraposing the two vital functions of the counter electrode catalyst, collecting electrons and catalyzing I-3(-) reduction, we propose a general strategy to understand the potential catalytic mechanism from the band structure and surface adsorption by using first-principles density functional theory (DFT) calculations. The theoretical investigations clearly indicate that the splendid catalytic performance originates from the zero band-gap of surface metal atoms and the surface chemical adsorption interaction between I-3(-) and exposed metal atoms. The proposed general strategy in this work for synthesizing a hybrid material with a unique network structure and understanding the catalytic mechanism of the electrocatalyst can guide the design of expected catalytic nanohybrids applied in various energy fields.

ROYAL SOC CHEMISTRY2019

Chargement

Investigation of interactions in two-dimensional electron gases with angular resolved photoemission spectroscopy

Carola Strasser

EPFL2015