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Lukas M. Bongartz

Publications and source records attributed to Lukas M. Bongartz.

4 recordsLinked to original sources

Statistical mechanics for organic mixed conductors: phase transitions in a lattice gas

Organic mixed conductors (OMCs) represent a promising class of materials for applications in bioelectronics, physical computing, and thermoelectrics. Rather unparalleled, OMCs feature dynamics spanning multiple length and time scales, involving an intricate coupling between electronic, ionic, and mass transport. These characteristics set them notably apart from traditional semiconductors and hinder the description by conventional semiconductor theory. In this work, we approach the charge carrier modulation of OMCs using statistical mechanics. We discuss OMCs from a thermodynamic perspective and contrast them with established semiconductor materials, highlighting key differences in their collective charge carrier dynamics. This motivates our description of OMCs as a lattice gas, which we analyze within the grand canonical ensemble. The model exhibits a first-order phase transition analogous to a classical vapor$\unicode{x2013}$liquid transition, governed by temperature and chemical potential. In doing so, it captures the formation of distinct low- and high-density carrier phases, consistent with recently reported experimental observations. It also illustrates how metastability near the phase boundary can give rise to history-dependent characteristics in device operation, a similarly well-reported effect in OMC transistors. This work is intended as a simple motivation for studying OMCs through the lens of statistical mechanics, offering a more natural description than traditional semiconductor models developed for materials of fundamentally distinct character.

cond-mat.dis-nn↗

Electron-Ion Coupling Breaks Energy Symmetry in Bistable Organic Electrochemical Transistors

Organic electrochemical transistors are extensively studied for applications ranging from bioelectronics to analog and neuromorphic computing. Despite significant advances, the fundamental interactions between the polymer semiconductor channel and the electrolyte, which critically determine the device performance, remain underexplored. Here, we examine the coupling between the benchmark semiconductor PEDOT:PSS and an ionic liquid to explain the bistable and non-volatile behavior observed in OECTs. Using X-ray scattering and spectroscopy techniques, we demonstrate how the electrolyte modifies the channel composition, enhances molecular order, and reshapes the energetic landscape. Notably, the observed bistability arises from asymmetric and path-dependent energetics during doping and dedoping, resulting in two distinct paths, driven by a direct interaction between the electronic and ionic charge carriers. These findings highlight the electrolyte's role in tuning charge carrier dynamics, positioning it as a powerful yet underutilized lever for enabling novel device functionalities.

cond-mat.mtrl-sci↗

Bistable Organic Electrochemical Transistors: Enthalpy vs. Entropy

Organic electrochemical transistors (OECTs) underpin a range of emerging technologies, from bioelectronics to neuromorphic computing, owing to their unique coupling of electronic and ionic charge carriers. In this context, various OECT systems exhibit significant hysteresis in their transfer curve, which is frequently leveraged to achieve non-volatility. Meanwhile, a general understanding of its physical origin is missing. Here, we introduce a thermodynamic framework that readily explains the emergence of bistable OECT operation via the interplay of enthalpy and entropy. We validate this model through temperature-resolved characterizations, material manipulation, and thermal imaging. Further, we reveal deviations from Boltzmann statistics for the subthreshold swing and reinterpret existing literature. Capitalizing on these findings, we finally demonstrate a single-OECT Schmitt trigger, thus compacting a multi-component circuit into a single device. These insights provide a fundamental advance for OECT physics and its application in non-conventional computing, where symmetry-breaking phenomena are pivotal to unlock new paradigms of information processing.

physics.app-ph↗

Brightening of Long, Polymer-Wrapped Carbon Nanotubes by sp$^{3}$ Functionalization in Organic Solvents

The functionalization of semiconducting single-walled carbon nanotubes (SWNTs) with sp$^{3}$ defects that act as luminescent exciton traps is a powerful means to enhance their photoluminescence quantum yield (PLQY) and to add optical properties. However, the synthetic methods employed to introduce these defects are so far limited to aqueous dispersions of surfactant-coated SWNTs, often with short tube lengths, residual metallic nanotubes and poor film formation properties. In contrast to that, dispersions of polymer-wrapped SWNTs in organic solvents feature unrivaled purity, higher PLQY and are easily processed into thin films for device applications. Here, we introduce a simple and scalable phase-transfer method to solubilize diazonium salts in organic nonhalogenated solvents for the controlled reaction with polymer-wrapped SWNTs to create luminescent aryl defects. Absolute PLQY measurements are applied to reliably quantify the defect-induced brightening. The optimization of defect density and trap depth results in PLQYs of up to 4 % with 90 % of photons emitted through the defect channel. We further reveal the strong impact of initial SWNT quality and length on the relative brightening by sp$^{3}$ defects. The efficient and simple production of large quantities of defect-tailored polymer-sorted SWNTs enables aerosol-jet printing and spin-coating of thin films with bright and nearly reabsorption-free defect emission, which are desired for carbon nanotube-based near-infrared light-emitting devices.

physics.app-ph↗