Dilara Meli

Northwestern University

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Jonathan Rivnay

Northwestern University

Bryan D. Paulsen

University of Notre Dame

Ruiheng Wu

Brunel University of London

Joseph Strzalka

Argonne National Laboratory

Iain McCulloch

University of Oxford

Simone Fabiano

Linköping University

Joshua Tropp

Texas Tech University

Karl J. Thorley

University of Kentucky

Adam Marks

Stanford University

Xudong Ji

Northwestern University

Cooperative Institutions

Northwestern University

University of Oxford

King Abdullah University of Science and Technology

Imperial College London

University of Michigan–Ann Arbor

Linköping University

University of Cambridge

Queen Mary University of London

Centre National de la Recherche Scientifique

Transnational Press London

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Ultraflexible and Stretchable Intrafascicular Peripheral Nerve Recording Device with Axon‐Dimension, Cuff‐Less Microneedle Electrode Array

Small (2022)

Dongxiao Yan Ahmad A. Jiman Elizabeth C. Bottorff Paras R. Patel Dilara Meli

Abstract Peripheral nerve mapping tools with higher spatial resolution are needed to advance systems neuroscience, and potentially provide a closed‐loop biomarker in neuromodulation applications. Two critical challenges of microscale neural interfaces are 1) how to apply them to small peripheral nerves, and 2) how to minimize chronic reactivity. A flexible microneedle nerve array (MINA) is developed, which is the first high‐density penetrating electrode array made with axon‐sized silicon microneedles embedded in low‐modulus thin silicone. The design, fabrication, acute recording, and chronic reactivity to an implanted MINA, are presented. Distinctive units are identified in the rat peroneal nerve. The authors also demonstrate a long‐term, cuff‐free, and suture‐free fixation manner using rose bengal as a light‐activated adhesive for two time‐points. The tissue response is investigated at 1‐week and 6‐week time‐points, including two sham groups and two MINA‐implanted groups. These conditions are quantified in the left vagus nerve of rats using histomorphometry. Micro computed tomography (micro‐CT) is added to visualize and quantify tissue encapsulation around the implant. MINA demonstrates a reduction in encapsulation thickness over previously quantified interfascicular methods. Future challenges include techniques for precise insertion of the microneedle electrodes and demonstrating long‐term recording.

10.1002/smll.202200311

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Citations (19)

Organic mixed conductors for electrochemical transistors

Matter (2023)

Joshua Tropp Dilara Meli Jonathan Rivnay

Bioelectronics

Neuromorphic engineering

Leverage (statistics)

Organic Electronics

10.1016/j.matt.2023.05.001

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Citations (48)

From p‐ to n‐Type Mixed Conduction in Isoindigo‐Based Polymers through Molecular Design

Advanced Materials (2022)

Zachary S. Parr Jorge Borges‐González Reem B. Rashid Karl J. Thorley Dilara Meli

Organic mixed ionic and electronic conductors are of significant interest for bioelectronic applications. Here, three different isoindigoid building blocks are used to obtain polymeric mixed conductors with vastly different structural and electronic properties which can be further fine-tuned through the choice of comonomer unit. This work shows how careful design of the isoindigoid scaffold can afford highly planar polymer structures with high degrees of electronic delocalization, while subtle structural modifications can control the dominant charge carrier (hole or electron) when probed in organic electrochemical transistors. A combination of experimental and computational techniques is employed to probe electrochemical, structural, and mixed ionic and electronic properties of the polymer series which in turn allows the derivation of important structure-property relations for this promising class of materials in the context of organic bioelectronics. Ultimately, these findings are used to outline robust molecular-design strategies for isoindigo-based mixed conductors that can support efficient p-type, n-type, and ambipolar transistor operation in an aqueous environment.

Ambipolar diffusion

Bioelectronics

Organic Electronics

Organic semiconductor

10.1002/adma.202107829

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Citations (58)

The effect of residual palladium on the performance of organic electrochemical transistors

Nature Communications (2022)

Sophie Griggs Adam Marks Dilara Meli Gonzague Rebetez Olivier Bardagot

Organic electrochemical transistors are a promising technology for bioelectronic devices, with applications in neuromorphic computing and healthcare. The active component enabling an organic electrochemical transistor is the organic mixed ionic-electronic conductor whose optimization is critical for realizing high-performing devices. In this study, the influence of purity and molecular weight is examined for a p-type polythiophene and an n-type naphthalene diimide-based polymer in improving the performance and safety of organic electrochemical transistors. Our preparative GPC purification reduced the Pd content in the polymers and improved their organic electrochemical transistor mobility by ~60% and 80% for the p- and n-type materials, respectively. These findings demonstrate the paramount importance of removing residual Pd, which was concluded to be more critical than optimization of a polymer's molecular weight, to improve organic electrochemical transistor performance and that there is readily available improvement in performance and stability of many of the reported organic mixed ionic-electronic conductors.

Organic Electronics

Bioelectronics

Organic semiconductor

10.1038/s41467-022-35573-y

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Citations (48)

Synthetic Nuances to Maximize n-Type Organic Electrochemical Transistor and Thermoelectric Performance in Fused Lactam Polymers

Journal of the American Chemical Society (2022)

Adam Marks Xingxing Chen Ruiheng Wu Reem B. Rashid Wen‐Long Jin

A series of fully fused n-type mixed conduction lactam polymers p(g7NCnN), systematically increasing the alkyl side chain content, are synthesized via an inexpensive, nontoxic, precious-metal-free aldol polycondensation. Employing these polymers as channel materials in organic electrochemical transistors (OECTs) affords state-of-the-art n-type performance with p(g7NC10N) recording an OECT electron mobility of 1.20 × 10-2 cm2 V-1 s-1 and a μC* figure of merit of 1.83 F cm-1 V-1 s-1. In parallel to high OECT performance, upon solution doping with (4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl)dimethylamine (N-DMBI), the highest thermoelectric performance is observed for p(g7NC4N), with a maximum electrical conductivity of 7.67 S cm-1 and a power factor of 10.4 μW m-1 K-2. These results are among the highest reported for n-type polymers. Importantly, while this series of fused polylactam organic mixed ionic-electronic conductors (OMIECs) highlights that synthetic molecular design strategies to bolster OECT performance can be translated to also achieve high organic thermoelectric (OTE) performance, a nuanced synthetic approach must be used to optimize performance. Herein, we outline the performance metrics and provide new insights into the molecular design guidelines for the next generation of high-performance n-type materials for mixed conduction applications, presenting for the first time the results of a single polymer series within both OECT and OTE applications.

Figure of Merit

10.1021/jacs.2c00735

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Citations (92)

The hole truth

Nature Materials (2023)

Ruiheng Wu Dilara Meli Jonathan Rivnay

10.1038/s41563-023-01643-9

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Citations (3)

Lactone Backbone Density in Rigid Electron‐Deficient Semiconducting Polymers Enabling High n‐type Organic Thermoelectric Performance

Angewandte Chemie (2021)

Maryam Alsufyani Marc‐Antoine Stoeckel Xingxing Chen Karl J. Thorley Rawad K. Hallani

Abstract Three lactone‐based rigid semiconducting polymers were designed to overcome major limitations in the development of n‐type organic thermoelectrics, namely electrical conductivity and air stability. Experimental and theoretical investigations demonstrated that increasing the lactone group density by increasing the benzene content from 0 % benzene (P‐0), to 50 % (P‐50), and 75 % (P‐75) resulted in progressively larger electron affinities (up to 4.37 eV), suggesting a more favorable doping process, when employing (N‐DMBI) as the dopant. Larger polaron delocalization was also evident, due to the more planarized conformation, which is proposed to lead to a lower hopping energy barrier. As a consequence, the electrical conductivity increased by three orders of magnitude, to achieve values of up to 12 S cm and Power factors of 13.2 μWm −1 K −2 were thereby enabled. These findings present new insights into material design guidelines for the future development of air stable n‐type organic thermoelectrics.

Organic semiconductor

Electron Mobility

10.1002/ange.202113078

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Citations (13)

On the fundamentals of organic mixed ionic/electronic conductors

Journal of Materials Chemistry C (2023)

Simone Fabiano Lucas Q. Flagg Tania C. Hidalgo Sahika Inal Loren G. Kaake

This perspective offers insights from discussions conducted during the Telluride Science meeting on organic mixed ionic and electronic conductors, outlining the challenges associated with understanding the behavior of this intriguing materials class.

Telluride

Electronic materials

10.1039/d3tc03058j

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Citations (9)

Influence of the molecular weight and size distribution of PSS on mixed ionic-electronic transport in PEDOT:PSS

Polymer Chemistry (2022)

Chun‐Yuan Lo Yuhang Wu Elorm Awuyah Dilara Meli Dan My Nguyen

The commercially available polyelectrolyte complex poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is ubiquitous in organic and hybrid electronics. As such, it has often been used as a benchmark material for fundamental studies and the development of new electronic devices. Yet, most studies on PEDOT:PSS have focused on its electronic conductivity in dry environments, with less consideration given to its ion transport, coupled ionic-electronic transport, and charge storage properties in aqueous environments. These properties are essential for applications in bioelectronics (sensors, actuators), charge storage devices, and electrochromic displays. Importantly, past studies on mixed ionic-electronic transport in PEDOT:PSS neglected to consider how the molecular structure of PSS affects mixed ionic-electronic transport. Herein, we therefore investigated the effect of the molecular weight and size distribution of PSS on the electronic properties and morphology of PEDOT:PSS both in dry and aqueous environments, and overall performance in organic electrochemical transistors (OECTs). Using reversible addition-fragmentation chain transfer (RAFT) polymerization with two different chain transfer agents, six PSS samples with monomodal, narrow (

10.1039/d2py00271j

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Citations (36)

Side chain engineering in indacenodithiophene-co-benzothiadiazole and its impact on mixed ionic–electronic transport properties

Journal of Materials Chemistry C (2024)

Isabelle Holzer Vincent Lemaur Meng Wang Hanyan Wu Lu Zhang

This well-studied polymer system does not conform to existing design criteria for imparting mixed conduction. The reasons for this anomalous behaviour are unravelled and used to outline more robust design criteria for new organic semiconductors.

Chain (unit)

10.1039/d3tc04738e

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Citations (1)