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커뮤니티
연구자들이 자신의 연구와 전문성을 널리 알리고, 새로운 협력의 기회를 만들 수 있는 네트워킹 공간이에요.
초록·키워드
Organic mixed ionic-electronic conducting polymers remain at the forefront of materials development for bioelectronic device applications. During electrochemical operation, structural dynamics and variations in electrostatic interactions in the polymer occur, which affect dual transport of the ions and electronic charge carriers. Such effects remain unclear due to a lack of <i>in situ</i> spectroscopic methods capable of capturing these dynamics, which hinders the rational design of higher-performance polymers. Herein, we present the first <i>in situ</i> transient absorption spectroelectrochemical measurement of a conducting polymer in the near-infrared, where photoexcited charge carrier dynamics are used to directly probe their nanoscale environment and trapping behavior in working electrodes. In this method, voltage is applied to charge or discharge the polymer, and the picosecond relaxation dynamics of directly photoexcited charge carriers are spectroscopically monitored to relate their location within the heterogeneous polymer nanostructure to their transport behavior. Applying this technique to working PEDOT:PSS electrodes, we investigated the impacts of voltage-induced changes in polymer chain packing and ion-carrier interactions on charge trapping. At lower voltages, carriers initially form within J-aggregated PEDOT chains that are deeply trapped due to strong electrostatic coupling to PSS<sup>-</sup> counterions. At higher voltages, the PEDOT lamellae expand and charge-ion pairs enter the PEDOT-rich domains, where trapping is decreased and carriers delocalize among the more tightly stacked, H-aggregated PEDOT chains. Further, this <i>in situ</i> spectroscopic method can also be more broadly applied to study electrochemical dynamics in accumulation-mode and n-type polymer electrodes and electrochemical transistors.
#Polaron
#Transient (computer programming)
#Ultrashort pulse
#In situ
#Ultrafast laser spectroscopy
#Absorption (acoustics)
#Materials science
#Polymer
#Analytical Chemistry (journal)
#Photochemistry
#Optoelectronics
#Chemical physics
#Chemistry
#Optics
#Physics
#Computer science
#Organic chemistry
#Composite material
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