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  1. Investigation of charge transfer in quantum dot (QD) systems is an area of great interest. Specifically, the relationship between capping ligand and rate of charge transfer has been studied as a means to optimize these materials. To investigate the role of ligand interaction on the QD surface for electron transfer, we designed and synthesized a series of ligands containing an electron accepting moiety, naphthalene bisimide (NBI). These ligands differ in their steric bulk: as one allows for π–π stacking between the NBI moieties at high surface coverages, while the other does not, allowing for a direct comparison of these effects. Once grafted onto QDs, these hybrid materials were studied using UV-Vis, fluorescence, and transient absorption spectroscopy. Interestingly, the sample with the fastest electron transfer was not the sample with the most NBI π–π stacking, it was instead where these ligands were mixed amongst oleic acid, breaking up H-aggregates between the NBI groups. 
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  2. Abstract

    Above‐equilibrium “hot”‐carrier generation in metals is a promising route to convert photons into electrical charge for efficient near‐infrared optoelectronics. However, metals that offer both hot‐carrier generation in the near‐infrared and sufficient carrier lifetimes remain elusive. Alloys can offer emergent properties and new design strategies compared to pure metals. Here, it is shown that a noble‐transition alloy, AuxPd1−x, outperforms its constituent metals concerning generation and lifetime of hot carriers when excited in the near‐infrared. At optical fiber wavelengths (e.g., 1550 nm), Au50Pd50provides a 20‐fold increase in the number of ≈0.8 eV hot holes, compared to Au, and a threefold increase in the carrier lifetime, compared to Pd. The discovery that noble‐transition alloys can excel at hot‐carrier generation reveals a new material platform for near‐infrared optoelectronic devices.

     
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  3. Abstract

    Mobilities and lifetimes of photogenerated charge carriers are core properties of photovoltaic materials and can both be characterized by contactless terahertz or microwave measurements. Here, the expertise from fifteen laboratories is combined to quantitatively model the current‐voltage characteristics of a solar cell from such measurements. To this end, the impact of measurement conditions, alternate interpretations, and experimental inter‐laboratory variations are discussed using a (Cs,FA,MA)Pb(I,Br)3halide perovskite thin‐film as a case study. At 1 sun equivalent excitation, neither transport nor recombination is significantly affected by exciton formation or trapping. Terahertz, microwave, and photoluminescence transients for the neat material yield consistent effective lifetimes implying a resistance‐free JV‐curve with a potential power conversion efficiency of 24.6 %. For grainsizes above ≈20 nm, intra‐grain charge transport is characterized by terahertz sum mobilities of ≈32 cm2V−1s−1. Drift‐diffusion simulations indicate that these intra‐grain mobilities can slightly reduce the fill factor of perovskite solar cells to 0.82, in accordance with the best‐realized devices in the literature. Beyond perovskites, this work can guide a highly predictive characterization of any emerging semiconductor for photovoltaic or photoelectrochemical energy conversion. A best practice for the interpretation of terahertz and microwave measurements on photovoltaic materials is presented.

     
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