石井 久夫

Organic multilayer systems, which are stacked layers of different organic materials, are used in various organic electronic devices such as organic light-emitting diodes (OLEDs) and organic field-effect transistors (OFETs). In particular, OFETs are promising as key components in flexible electronic devices. In this study, we investigated how the inclusion of an insulating tetratetracontane (TTC) interlayer in ambipolar indigo-based OFETs can be used to alter the crystallinity and electrical properties of the indigo charge transport layer. We find that the inclusion of a 20-nm-thick TTC film thermally annealed at a low temperature of 70 °C acts to significantly increase the ambipolar electrical transport of the indigo layer. X-ray diffraction, atomic force microscopy, and vibrational sum frequency generation measurements showed that annealing the TTC film significantly improved its ordering. The electronic sum-frequency generation spectra of TTC/indigo bilayers show that this improved ordering of TTC films promotes the growth of crystalline indigo films that exhibit charge mobilities in OFET that are nearly an order of magnitude larger than those measured for devices grown on unannealed TTC layers. Furthermore, using vibrational sum-frequency generation spectroscopy, we found that pre-annealing the TTC layer prior to indigo deposition can suppress the formation of defects within the TTC layer during indigo film growth, which also contributes to enhanced charge transport. Our results highlight the importance of controlling the molecular ordering within the interlayer contacts in OFET structures to achieve an enhanced performance.

Illumination stress (IS) and negative bias under illumination stress (NBIS) cause considerable device instability in thin-film transistors based on amorphous In–Ga–Zn–O (a-IGZO). Models using in-gap states are suggested to explain device instability. Therefore, to provide reliably their density of states (DOS), this study investigated the valence band, conduction band, and in-gap states of an a-IGZO thin film. The DOS of in-gap states was directly determined in a dynamic range of six orders of magnitude through constant final state yield spectroscopy (CFS-YS) using low-energy and low-flux photons. Furthermore, light irradiation irreversibly induced extra in-gap states near the Fermi level and shifted the Fermi level to the vacuum level side, which should be related to the device instability due to IS and NBIS. Hard x-ray photoemission spectroscopy and ultraviolet photoemission spectroscopy using synchrotron radiation observed the large DOS of in-gap states near the Fermi level as in previous works. Here, we reveal that they are not intrinsic electronic states of undamaged a-IGZO, but induced by the intense measurement light of synchrotron radiation. This study demonstrates that CFS-YS is useful for determining the reliable DOS of the in-gap states for samples that are sensitive to light irradiation. The absorption spectrum measured through photothermal deflection spectroscopy is interpreted based on DOS directly determined via photoemission spectroscopies. This indicates that the line shape in the energy region below the region assigned to the Urbach tail in previous works actually roughly reflects the DOS of occupied in-gap states.