The development of transistors with high gain is essential for applications ranging from switching elements and drivers to transducers for chemical and biological sensing. Organic transistors have become well-established based on their distinct advantages, including ease of fabrication, synthetic freedom for chemical functionalization, and the ability to take on unique form factors. These devices, however, are largely viewed as belonging to the low-end of the performance spectrum. Here we present organic electrochemical transistors with a transconductance in the mS range, outperforming transistors from both traditional and emerging semiconductors. The transconductance of these devices remains fairly constant from DC up to a frequency of the order of 1 kHz, a value determined by the process of ion transport between the electrolyte and the channel. These devices, which continue to work even after being crumpled, are predicted to be highly relevant as transducers in biosensing applications.
Poly(3,4-ethylenedioxythiophene) doped with poly(styrenesulfonate), PEDOT:PSS, has been utilized for over two decades as a stable, solution-processable hole conductor. While its hole transport properties have been the subject of intense investigation, recent work has turned to PEDOT:PSS as a mixed ionic/electronic conductor in applications including bioelectronics, energy storage and management, and soft robotics. Conducting polymers can efficiently transport both holes and ions when sufficiently hydrated, however, little is known about the role of morphology on mixed conduction. Here, we show that bulk ionic and electronic mobilities are simultaneously affected by processing-induced changes in nano- and meso-scale structure in PEDOT:PSS films. We quantify domain composition, and find that domain purification on addition of dispersion co-solvents limits ion mobility, even while electronic conductivity improves. We show that an optimal morphology allows for the balanced ionic and electronic transport that is critical for prototypical mixed conductor devices. These findings may pave the way for the rational design of polymeric materials and processing routes to enhance devices reliant on mixed conduction.
Trap-assisted recombination, despite
being lower as compared with traditional inorganic solar cells, is
still the dominant recombination mechanism in perovskite solar cells
(PSCs) and limits their efficiency. We investigate the attributes
of the primary trap-assisted recombination channels (grain boundaries
and interfaces) and their correlation to defect ions in PSCs. We achieve
this by using a validated device model to fit the simulations to the
experimental data of efficient vacuum-deposited p–i–n
and n–i–p CH3NH3PbI3 solar cells, including the light intensity dependence of the open-circuit
voltage and fill factor. We find that, despite the presence of traps
at interfaces and grain boundaries (GBs), their neutral (when filled
with photogenerated charges) disposition along with the long-lived
nature of holes leads to the high performance of PSCs. The sign of
the traps (when filled) is of little importance in efficient solar
cells with compact morphologies (fused GBs, low trap density). On
the other hand, solar cells with noncompact morphologies (open GBs,
high trap density) are sensitive to the sign of the traps and hence
to the cell preparation methods. Even in the presence of traps at
GBs, trap-assisted recombination at interfaces (between the transport
layers and the perovskite) is the dominant loss mechanism. We find
a direct correlation between the density of traps, the density of
mobile ionic defects, and the degree of hysteresis observed in the
current–voltage (J–V) characteristics. The presence of defect states or mobile ions not
only limits the device performance but also plays a role in the J–V hysteresis.
Electrolyte-gated organic transistors offer low bias operation facilitated by direct contact of the transistor channel with an electrolyte. Their operation mode is generally defined by the dimensionality of charge transport, where a field-effect transistor allows for electrostatic charge accumulation at the electrolyte/semiconductor interface, whereas an organic electrochemical transistor (OECT) facilitates penetration of ions into the bulk of the channel, considered a slow process, leading to volumetric doping and electronic transport. Conducting polymer OECTs allow for fast switching and high currents through incorporation of excess, hygroscopic ionic phases, but operate in depletion mode. Here, we show that the use of glycolated side chains on a thiophene backbone can result in accumulation mode OECTs with high currents, transconductance, and sharp subthreshold switching, while maintaining fast switching speeds. Compared with alkylated analogs of the same backbone, the triethylene glycol side chains shift the mode of operation of aqueous electrolyte-gated transistors from interfacial to bulk doping/transport and show complete and reversible electrochromism and high volumetric capacitance at low operating biases. We propose that the glycol side chains facilitate hydration and ion penetration, without compromising electronic mobility, and suggest that this synthetic approach can be used to guide the design of organic mixed conductors.organic electronics | electrochemical transistor | semiconducting polymers
Thin-film photovoltaics is a promising technology for low-cost and sustainable renewable energy sources. Organic-inorganic (hybrid) lead halide perovskite solar cells have recently aroused wide interest in photovoltaic applications because of their impressive power conversion efficiencies (PCEs), now exceeding 21%. [1][2][3] Importantly, the perovskite thin-film absorber can be deposited using low-cost and abundant starting materials, hence with a large potential for the preparation of inexpensive photovoltaic devices. 4 The high PCEs are the result of the very high absorption coefficient and mobilities of the photogenerated electrons and holes
The organic electrochemical
transistor (OECT), capable of transducing
small ionic fluxes into electronic signals in an aqueous environment,
is an ideal device to utilize in bioelectronic applications. Currently,
most OECTs are fabricated with commercially available conducting poly(3,4-ethylenedioxythiophene)
(PEDOT)-based suspensions and are therefore operated in depletion
mode. Here, we present a series of semiconducting polymers designed
to elucidate important structure–property guidelines required
for accumulation mode OECT operation. We discuss key aspects relating
to OECT performance such as ion and hole transport, electrochromic
properties, operational voltage, and stability. The demonstration
of our molecular design strategy is the fabrication of accumulation
mode OECTs that clearly outperform state-of-the-art PEDOT-based devices,
and show stability under aqueous operation without the need for formulation
additives and cross-linkers.
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