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Marin Rusu

Publications and source records attributed to Marin Rusu.

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Photovoltaic potential of tin perovskites revealed through layer-by-layer investigation of optoelectronic and charge transport properties

Tin perovskites are the most promising environmentally friendly alternative to lead perovskites. Among tin perovskites, FASnI3 (CH4N2SnI3) shows optimum band gap, and easy processability. However, the performance of FASnI3 based solar cells is incomparable to lead perovskites for several reasons, including energy band mismatch between the perovskite absorber film and the charge transporting layers (CTLs) for both types of carriers, i.e., for electrons (ETLs) and holes (HTLs). However, the band diagrams in the literature are inconsistent, and the charge extraction dynamics are poorly understood. In this paper, we study the energy band positions of FASnI3 based perovskites using Kelvin probe (KP) and photoelectron yield spectroscopy (PYS) to provide a precise band diagram of the most used device stack. In addition, we analyze the defects within the current energetic landscape of tin perovskites. We uncover the role of bathocuproine (BCP) in enhancing the electron extraction at the fullerene C60/BCP interface. Furthermore, we used transient surface photovoltage (tr-SPV) for the first time for tin perovskites to understand the charge extraction dynamics of the most reported HTLs such as NiOx and PEDOT, and ETLs such as C60, ICBA, and PCBM. Finally, we used Hall effect, KP, and time-resolved photoluminescence (TRPL) to estimate an accurate value of the p-doping concentration in FASnI3 and showed a consistent result of 1.5 * 1017 cm-3. Our findings prove that the energetic system of tin halide perovskites is deformed and should be redesigned independently from lead perovskites to unlock the full potential of tin perovskites.

cond-mat.mtrl-sci

Fast near-infrared photodetectors based on nontoxic and solution-processable AgBiS2

Solution-processable near-infrared (NIR) photodetectors are urgently needed for a wide range of next-generation electronics, including sensors, optical communications and bioimaging. However, there is currently a compromise between low toxicity and slow (<300 kHz cut-off frequency) organic materials versus faster detectors (>300 kHz cut-off frequency) based on compounds containing toxic lead or cadmium. Herein, we circumvent this trade-off by developing solution-processed AgBiS2 photodetectors with high cut-off frequencies under both white light (>1 MHz) and NIR (approaching 500 kHz) illumination. These high cut-off frequencies are due to the short transit distances of charge-carriers in the AgBiS2 photodetectors, which arise from the strong light absorption of these materials, such that film thicknesses well below 120 nm are adequate to absorb >65% of near-infrared to visible light. By finely controlling the thickness of the photoactive layer, we can modulate the charge-collection efficiency, achieve low dark current densities, and minimize the effects of ion migration to realize fast photodetectors that are stable in air. These outstanding characteristics enable real-time heartbeat sensors based on NIR AgBiS2 photodetectors. # equal contribution, * corresponding authors

cond-mat.mtrl-sci

Understanding the growth mechanism of BaZrS$_3$ chalcogenide perovskite thin films from sulfurized oxide precursors

Barium zirconium sulfide (BaZrS3) is an earth-abundant and environmentally friendly chalcogenide perovskite with promising properties for various energy conversion applications. Recently, sulfurization of oxide precursors has been suggested as a viable solution for effective synthesis, especially from the perspective of circumventing the difficulty of handling alkali earth metals. In this work, we explore in detail the synthesis of BaZrS3 from Ba-Zr-O oxide precursor films sulfurized at temperatures ranging from 700 °C to 1000 °C. We propose a formation mechanism of BaZrS3 based on a two-step reaction involving an intermediate amorphization step of the BaZrO3 crystalline phase. We show how the diffusion of sulfur (S) species in the film is the rate-limiting step of this reaction. The processing temperature plays a key role in determining the total fraction of conversion from oxide to sulfide phase at a constant flow rate of the sulfur-containing H2S gas used as a reactant. Finally, we observe the formation of stoichiometric BaZrS3 (1:1:3), even under Zr-rich precursor conditions, with the formation of ZrO2 as a secondary phase. This marks BaZrS3 quite unique among the other types of chalcogenides, such as chalcopyrites and kesterites, which can instead accommodate quite a large range of non-stoichiometric compositions. This work opens up a pathway for further optimization of the BaZrS3 synthesis process, straightening the route towards future applications of this material.

cond-mat.mtrl-sci

Water adsorption enhances electrical conductivity in transparent p-type CuI

CuI has been recently rediscovered as a p-type transparent conductor with a high figure of merit. Even though many metal iodides are hygroscopic, the effect of moisture on the electrical properties of CuI has not been clarified. In this work, we observe a two-fold increase in the conductivity of CuI after exposure to ambient humidity for 5 hours, followed by slight long-term degradation. Simultaneously, the work function of CuI decreases by almost 1 eV, which can explain the large spread in the previously reported work function values. The conductivity increase is partially reversible and is maximized at intermediate humidity levels. Based on the large intra-grain mobility measured by THz spectroscopy, we suggest that hydration of grain boundaries may be beneficial for the overall hole mobility.

physics.app-ph

Preparation and Characterization of Metal-free graphitic Carbon Nitride Film Photocathodes for Light-induced Hydrogen Evolution

Very recently, it has been shown that an abundant material, polymeric carbon nitride, can produce hydrogen from water under visible-light irradiation in the presence of a sacrificial donor [1]. We will present here the preparation and characterization of graphitic carbon nitride (g-C3N4) films on semiconducting substrates by thermal condensation of dicyandiamide precursor under inert gas conditions. Structural and surface morphological studies of the carbon nitride films suggest a high porosity of g-C3N4 thin film consisting of a network of nanocrystallites. Photo-electrochemical investigations show upon cathodic polarization light-induced hydrogen evolution for a wide range of proton concentrations in the aqueous electrolyte. Additionally, Synchrotron radiation based photoelectron spectroscopy has been applied to study the surface/near-surface chemical composition of the utilized g-C3N4 film photocathodes. For the first time it is shown that g-C3N4 films can be successfully applied as photoelectrochemical material for light induced hydrogen evolution. [1]X. Wang, K. Maeda, A. Thomas, K. Takanabe, G. Xin, J. M. Carlsson, K. Domen, M. Antonietti, Nature Mat. 2009, 8, 76-80.

physics.chem-ph