May 2024
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6 Reads
Analytical Chemistry
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May 2024
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6 Reads
Analytical Chemistry
March 2024
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6 Reads
MRS Communications
November 2023
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14 Reads
Perovskites have emerged as a forerunner of electronics research due to their vast potential for optoelectronic applications. The numerous combinations of constituent ions and the potential for doping of perovskites lead to a high demand to track the underlying electronic properties. Solution‐based electrochemistry is particularly promising for detailed and facile assessment of perovskites. Here, electrochemical impedance spectroscopy (EIS) of methylammonium lead iodide (MAPbI3) thin films is performed and model them with an equivalent circuit that accounts for solvent, ionic, and thin film effects. A dielectric constant consistent with prior AC studies and a diffusion constant harmonious with cation motion in MAPbI3 are extracted. An electrical double layer thickness in the perovskite film of 54 nm is obtained, consistent with lithium doping in perovskite films. Comparing the EIS and equivalent circuit model of perovskite films to control ITO‐only data enabled the assignment of the ions at each interface. This comparison implied a double layer of primarily lithium ions inside the perovskite film at the solution interface with significant recombination of ions on the solution side of the interface. This demonstrates EIS as a powerful tool for studying the fundamental charge accumulation and transport processes in perovskite thin films.
November 2023
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25 Reads
DNA helicase activity is essential for the vital DNA metabolic processes of recombination, replication, transcription, translation, and repair. Recently, an unexpected, rapid exponential ATP‐stimulated DNA unwinding rate was observed from an Archaeoglobus fulgidus helicase (AfXPB) as compared to the slower conventional helicases from Sulfolobus tokodaii, StXPB1 and StXPB2. This unusual rapid activity suggests a “molecular wrench” mechanism arising from the torque applied by AfXPB on the duplex structure in transitioning from open to closed conformations. However, much remains to be understood. Here, we investigate the concentration dependence of DNA helicase binding and ATP‐stimulated kinetics of StXPB2 and AfXPB, as well as their binding and activity in Bax1 complexes, via an electrochemical assay with redox‐active DNA monolayers. StXPB2 ATP‐stimulated activity is concentration‐independent from 8 to 200 nM. Unexpectedly, AfXPB activity is concentration‐dependent in this range, with exponential rate constants varying from seconds at concentrations greater than 20 nM to thousands of seconds at lower concentrations. At 20 nM, rapid exponential signal decay ensues, linearly reverses, and resumes with a slower exponential decay. This change in AfXPB activity as a function of its concentration is rationalized as the crossover between the fast molecular wrench and slower conventional helicase modes. AfXPB‐Bax1 inhibits rapid activity, whereas the StXPB2‐Bax1 complex induces rapid kinetics at higher concentrations. This activity is rationalized with the crystal structures of these complexes. These findings illuminate the different physical models governing molecular wrench activity for improved biological insight into a key factor in DNA repair.
November 2023
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20 Reads
MRS Communications
Hybrid perovskites have attracted great interest in solar energy conversion and optoelectronic applications. The interconnected ionic and electronic effects complicate assessing the underlying electrical processes while contributing greatly to the efficiency and stability of devices. Fortunately, these coupled processes manifest on distinct timescales that enable frequency-specific electrochemical analysis. However, hybrid perovskites dissolve in most of the common aqueous and organic solvents utilized for electrochemistry. Here, we utilize a hydrofluoroether (HFE) solvent toolkit to perform nondestructive electrochemical impedance spectroscopy of methylammonium lead iodide (MAPbI3) perovskite thin films. This enables the extraction of dielectric constants and double-layer formation in these perovskite films.
April 2023
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108 Reads
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4 Citations
ACS Materials Letters
April 2023
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199 Reads
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11 Citations
Perovskite light‐emitting diodes (PeLEDs) are advancing because of their superior external quantum efficiencies (EQEs) and color purity. Still, additional work is needed for blue PeLEDs to achieve the same benchmarks as the other visible colors. This study demonstrates an extremely efficient blue PeLED with a 488 nm peak emission, a maximum luminance of 8600 cd m⁻², and a maximum EQE of 12.2% by incorporating the double‐sided ethane‐1,2‐diammonium bromide (EDBr2) ligand salt along with the long‐chain ligand methylphenylammonium chloride (MeCl). The EDBr2 successfully improves the interaction between 2D perovskite layers by reducing the weak van der Waals interaction and creating a Dion–Jacobson (DJ) structure. Whereas the pristine sample (without EDBr2) is inhibited by small stacking number (n) 2D phases with nonradiative recombination regions that diminish the PeLED performance, adding EDBr2 successfully enables better energy transfer from small n phases to larger n phases. As evidenced by photoluminescence (PL), scanning electron microscopy (SEM), and atomic force microscopy (AFM) characterization, EDBr2 improves the morphology by reduction of pinholes and passivation of defects, subsequently improving the efficiencies and operational lifetimes of quasi‐2D blue PeLEDs.
September 2022
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32 Reads
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2 Citations
ACS Applied Optical Materials
September 2022
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22 Reads
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10 Citations
Precision Engineering
The consistent motivation to observe molecular electronics and quantum effects drives the need for the tunable and robust fabrication of nanogap devices. Electron beam lithography (EBL) offers high fidelity fabrication to construct arrayed nanogaps, and methods have been developed to achieve sub-10 nm channel widths. However, many of these approaches involve multiple lithography steps or specialized techniques that limit throughput and universality. This work describes a simple, single EBL step, continuous dose, and direct feature write method of fabricating electrode pairs with nanogap spacing from 5 to 40 nm. This straightforward technique relies on precise electron beam focusing coupled with cold lithography for developing. Overall, this protocol enables efficient production of electrode nanogaps to facilitate the study of nanoscale materials and effects.
... [17,18] For example, Alahbakhshi et al. introduced the symmetric double-sided ethane-1,2-diammonium bromide (EDBr 2 ) into perovskite films to form DJ phase perovskite, which achieved stable sky blue emission at 488 nm. [19] EDBr 2 not only reduces the thickness of adjacent inorganic layers to improve the interaction between 2D inorganic layers but also regulates phase distribution to promote energy transfer. ...
April 2023
... Moreover, CsPbBr 3 has a high melting point of 570 • C and shows excellent resistance to light, heat, and degradation. Despite the rapid progress of CsPbBr 3 perovskite LECs, there are still some challenges that limit their practical applications [17][18][19]. ...
September 2022
ACS Applied Optical Materials
... However, it's relevant to note that top electrode sizes minimally impacts electric field generation, as demonstrated in our preliminary work in [18]. Hence, alternative methods such as atomic layer deposition and electron beam lithography could be considered for electrode patterning [34]- [36]. Overall, molFCN fabrication could rely on the combination of advanced lithographic processes and molecules self-assembling, possibly avoiding atomic-scale manipulation necessary for other QCA implementations [37], [38]. ...
September 2022
Precision Engineering