Deep traps can be desired, as in the case of plastic semiconductors used for memory devices, but they can also decrease the efficiency of the material to conduct electrical charges. In the case of solar cells, deep traps can decrease the efficiency of the conversion of light into electricity.

To further explore the deep trap phenomenon, a group of scientists led by Professors of Chemistry and Biochemistry Paul Barbara and Allen Bard developed a single-particle technique to study small portions of semiconductor material at the nanoscale.

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Organic field-effect transistors (OFETs) with polymer charge-trapping dielectric, which exhibit many advantages over Si-based memory devices such as low cost, light weight, and flexibility, still suffer challenges in practical application due to the unsatisfied endurance characteristics and even the lack of fundamental of behind mechanism. Here, we revealed that the degradation of endurance characteristics of pentacene OFET with poly(2-vinyl naphthalene) (PVN) as charge-storage layer is dominated by the deep hole-traps in PVN by using the photo-stimulated charge de-trapping technique with the fiber-coupled monochromatic-light probes. The depth distribution of hole-traps in PVN film of pentacene OFET is also provided.

The endurance characteristics of pentacene OFET with polymer charge-trapping layer is related with the trapping/de-trapping processes of charges in polymer during P/E operations under a set of applied negative/positive gate-pulses. If the number of holes de-trapped from polymer after an erasing operation under a positive gate-pulse is lower than that trapped in polymer after an initial programming operation under a negative gate pulse, the threshold voltage in the erasing transfer characteristics should be shifted to the left side of gate-voltage axis. The further increase of the number of un-removable holes in polymer during the following continuous erasing operation cycles will result in the further left-shift of threshold voltage in the erasing transfer characteristic curve of the OFET, as schematically shown by 'Ideg' in Fig. 1, leading to the difference between the drain current IDS-I electrically read from the curve Iinitial and the drain current IDS-deg electrically read from the curve Ideg as shown in Fig. 1, which is generally defined as the degradation of the endurance characteristics.

In this work, the un-removable holes trapped in polymer under a positive gate-pulse is revealed to be related with the deep hole-traps in polymer dielectric. In fact, the deep trapping centers in polymers have been identified corresponding to the chemical defects, such as oxidized groups, additives, impurities and adsorption of water molecules, etc. by using spectroscopic experimental techniques, such as the deep trap level of 4.97 eV in polyethylene (PE)14, 15. By analyzing the exciting photon-energy-dependent charge-de-trapping behavior, we point out that the degradation in the endurance characteristics of pentacene based OFET memory with PVN charge-storage layer is dominated by the deep hole-traps in PVN.

The third run of 200-P/E-operation-cycles of pentacene OFET was performed in the dark, as shown in region III of Fig. 5a, indicating a similar tendency in the P/E-operation-cycle dependence of the drain current with that shown in region I. The little increase of drain current during the first erasing operation should be ascribed to the fact that some of the traps with the depths of less than 1.95 eV occupied by holes after turning off the light can be removed under a positive gate pulse once more, leading to the right-side shift of erasing transfer curve of the OFET, thus an increase of drain current as read electrically. During the third run of 200-P/E-operation-cycles more holes are further trapped by the deeper traps with the depth of larger than 1.95 eV, resulting in the further left-shift of erasing transfer curve of pentacene OFET, thus the decrease at the minimum value of drain current IMin, as compared with that shown in region I in Fig. 5a. The fourth run of 200-P/E-operation-cycles was performed under the irradiation of 635-nm photon again, as shown in region IV of Fig. 5a. The similar tendency in the P/E-operation-cycle dependence of the drain current with those shown in regions II of Fig. 5a was observed, while the further decrease at the minimum of drain current IMin was recorded after the fourth run of 200-P/E-operation-cycles, as compared with that shown in region II in Fig. 5a. It means that during four continuous runs of 200-P/E-operation-cycles (800 P/E operation cycles) more and more holes were trapped by the deep traps with the depths of larger than 1.95 eV.

Four similar 200-P/E-operation-cycles runs were also performed on pentacene OFET by using a monochromatic light of 532 nm (61 mW/cm2), corresponding to a photon energy of 2.33 eV, as shown in Fig. 5b. In region II and IV of Fig. 5b, during the early P/E operation cycles the quick rise of drain current for pentacene OFET as electrically read may be ascribed to the low fiber-coupling efficiency of light source in our apparatus, which leads to more time needed for exciting all the holes trapped in deep traps with depths of less than 2.33 eV in PVN film. After the drain current reaches the maximum value IMax, it decreases monotonously with the increase of P/E operation cycles, similar with that shown in region II of Fig. 5a. The similar tendency in the P/E operation-cycle dependence of drain current during the following third and fourth runs of 200-P/E-operation-cycles with those shown in Fig. 5a can be observed. It means that the deeper traps with the depth of larger than 2.33 eV still exist in PVN film of pentacene OFET.

To verify our conclusion, Fig. 5c shows the erasing endurance characteristics during four runs of 200-P/E-operation-cycles performed on pentacene OFET by using a monochromatic light of 375 nm, corresponding to a photon energy of 3.31 eV (18 mW/cm2). During the second run of 200-P/E-operation-cycles, it takes more P/E-operation-cycles (or time) to reach the maximum value of drain current IMax under the irradiation of 375-nm photons than that under the irradiation of 532-nm photons as shown in Fig. 5b, and the maximum value of drain current IMax is near that during the first erasing operation for pentacene OFET without degradation, as shown in region I of Fig. 5c. It is worth noting that after reaching the maximum value IMax, the drain current of pentacene OFET under the irradiation of 375-nm photons still shows a slow monotonous decrease trend, as shown in regions II and IV of Fig. 5c. While the minimum value of drain current IMin for pentacene OFET after the fourth run of 200-P/E-operation-cycles is still a little lower than that after the second run of 200-P/E-operation-cycles. It means that the depth of the deepest hole-traps in PVN film of pentacene OFET is located around 3.31 eV, but there still exists other deeper traps with a low face density and a depth of larger than 3.31 eV in PVN film, which is temporarily unknown due to the lack of the monochromatic light source of less than 375 nm in our apparatus. Based on above experimental results, the trapping and de-trapping processes of holes in PVN film of pentacene OFET device can be schematically drawn by using Fig. 6a,b, respectively. After a programming operation by applying a negative gate pulse on pentacene OFET, holes in pentacene will be transferred to PVN and trapped in hole traps with different depths randomly. While after subsequent erasing operation those holes trapped in deep traps cannot be driven to pentacene layer by applying a positive gate pulse, and those holes trapped in deep traps only can be excited by using photon irradiation with an appropriate photon energy.

In summary, this work reveals the degradation mechanism of the endurance characteristics of pentacene OFET with PVN charge-trapping layer by using the photo-stimulated charge de-trapping technique. We found that the shift of Vth in the erasing transfer characteristics after a lot of P/E operation cycles should be ascribed to the hole-trapping in deep traps, in which the trapped holes cannot be de-trapped by applying a positive erasing gate pulse. Pentacene OFET with charge-trapping layer of shallow traps is desired to enhance its reliability for promoting its application in the future.

Abstract:In this study, the results of hydrogen plasma treatments of -Ga2O3, -Ga2O3, -Ga2O3 and -Ga2O3 polymorphs are analyzed. For all polymorphs, the results strongly suggest an interplay between donor-like hydrogen configurations and acceptor complexes formed by hydrogen with gallium vacancies. A strong anisotropy of hydrogen plasma effects in the most thermodynamically stable -Ga2O3 are explained by its low-symmetry monoclinic crystal structure. For the metastable, -, - and -polymorphs, it is shown that the net result of hydrogenation is often a strong increase in the density of centers supplying electrons in the near-surface regions. These centers are responsible for prominent, persistent photocapacitance and photocurrent effects. Keywords: Ga2O3; polymorphs; hydrogen; plasma; deep traps

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