Brohmann Maximilian, Wieland Sonja, Angstenberger Simon, Herrmann Niklas J, Lüttgens Jan, Fazzi Daniele, Zaumseil Jana
Institute for Physical Chemistry, Universität Heidelberg, D-69120 Heidelberg, Germany.
Centre for Advanced Materials, Universität Heidelberg, D-69120 Heidelberg, Germany.
ACS Appl Mater Interfaces. 2020 Jun 24;12(25):28392-28403. doi: 10.1021/acsami.0c05640. Epub 2020 Jun 11.
Photoswitchable, ambipolar field-effect transistors (FETs) are fabricated with dense networks of polymer-sorted, semiconducting single-walled carbon nanotubes (SWCNTs) in top-gate geometry with photochromic molecules mixed in the polymer matrix of the gate dielectric. Both hole and electron transport are strongly affected by the presence of spiropyran and its photoisomer merocyanine. A strong and persistent reduction of charge carrier mobilities and thus drain currents upon UV illumination (photoisomerization) and its recovery by annealing give these SWCNT transistors the basic properties of optical memory devices. Temperature-dependent mobility measurements and density functional theory calculations indicate scattering of charge carriers by the large dipoles of the merocyanine molecules and electron trapping by protonated merocyanine as the underlying mechanism. The direct dependence of carrier mobility on UV exposure is employed to pattern high- and low-resistance areas within the FET channel and thus to guide charge transport through the nanotube network along predefined paths with micrometer resolution. Near-infrared electroluminescence imaging enables the direct visualization of such patterned current pathways with good contrast. Elaborate mobility and thus current density patterns can be created by local optical switching, visualized and erased again by reverse isomerization through heating.
可光开关的双极场效应晶体管(FET)是采用聚合物分选的半导体单壁碳纳米管(SWCNT)密集网络,以顶栅结构制造而成,其中光致变色分子混入栅极电介质的聚合物基质中。空穴和电子传输都受到螺吡喃及其光异构体部花青的强烈影响。在紫外光照射(光异构化)时,电荷载流子迁移率以及漏极电流会大幅且持续降低,通过退火恢复,这些SWCNT晶体管具备了光存储器件的基本特性。与温度相关的迁移率测量和密度泛函理论计算表明,电荷载流子被部花青分子的大偶极子散射以及被质子化部花青捕获电子是其潜在机制。利用载流子迁移率对紫外光照射的直接依赖性,在FET沟道内形成高电阻和低电阻区域的图案,从而以微米级分辨率沿着预定路径引导电荷通过纳米管网络传输。近红外电致发光成像能够直接清晰地可视化这种图案化的电流路径。通过局部光开关可以创建精细的迁移率进而电流密度图案,通过加热进行反向异构化将其可视化并再次消除。