Solution-processed networks of semiconducting, single-walled carbon nanotubes (SWCNTs) have attracted considerable attention as materials for next-generation electronic devices and circuits. However, the impact of the SWCNT network composition on charge transport on a microscopic level remains an open and complex question. Here, we use charge-modulated absorption and photoluminescence spectroscopy to probe exclusively the mobile charge carriers in monochiral (6,5) and mixed SWCNT network field-effect transistors. Ground state bleaching and charge-induced trion absorption features, as well as exciton quenching are observed depending on applied voltage and modulation frequency. Through correlation of the modulated mobile carrier density and the optical response of the nanotubes, we find that charge transport in mixed SWCNT networks depends strongly on the diameter and thus bandgap of the individual species. Mobile charges are preferentially transported by small bandgap SWCNTs especially at low gate voltages, whereas large bandgap species only start to participate at higher carrier concentrations. Our results demonstrate the excellent suitability of modulation spectroscopy to investigate charge transport in nanotube network transistors and highlight the importance of SWCNT network composition for their performance.KEYWORDS single-walled carbon nanotubes, networks, charge transport, charge modulation spectroscopy,
photoluminescence, trionSemiconducting single-walled carbon nanotubes (SWCNTs) have emerged as a promising material for future electronic applications as they combine high charge carrier mobilities with mechanical flexibility and solution-processability. 1, 2 Stimulated by the major progress in sorting techniques such as gel chromatography, 3, 4 density gradient ultracentrifugation, 5 aqueous two-phase separation, 6 and polymer-wrapping, 7-9 the reproducible fabrication of highperformance field-effect transistors (FETs) and circuits based on networks of purely semiconducting SWCNTs has become feasible. [10][11][12][13][14][15][16] Nonetheless, charge transport in nanotube networks is not yet fully understood especially regarding mixed networks of nanotube species with varying compositions. 17, 18 A detailed understanding of the fundamental transport parameters is necessary to further optimize effective carrier mobilities for competitive network devices at a minimum cost for purification.Charge transport in semiconductors is commonly studied through temperature-dependent measurements of conductivities and carrier mobilities. 17, 19-21 However, these techniques cannot distinguish between different SWCNT species and thus are not suitable to examine the chirality-dependent contributions to the macroscopic device performance. Given the high sensitivity of SWCNT absorption and emission features to charge carriers, which was shown in several studies, 22-25 electro-optical methods could provide additional and even chiralityspecific insights. For example, based on the analysis of the E11 absorption band change of...