Influence of the dielectric constant of a polyvinyl phenol insulator on the field-effect mobility of a pentacene-based thin-film transistor Yunseok Jang, Do Hwan Kim, Yeong Don Park, Jeong Ho Cho, Minkyu Hwang, and Kilwon Cho Citation: Applied Physics Letters 87, 152105 (2005); doi: 10.1063/1.2093940 View online: http://dx.doi.org/10.1063/1.2093940 View Table of Contents: http://scitation.aip.org/content/aip/journal/apl/87/15?ver=pdfcov Published by the AIP Publishing Articles you may be interested in Effects of the permanent dipoles of self-assembled monolayer-treated insulator surfaces on the field-effect mobility of a pentacene thin-film transistor Appl. Phys. Lett. 90, 132104 (2007); 10.1063/1.2457776 Pentacene-based thin film transistors with titanium oxide-polystyrene/polystyrene insulator blends: High mobility on high K dielectric films Appl. Phys. Lett. 90, 062111 (2007); 10.1063/1.2450660 Field-effect mobility of polycrystalline tetrabenzoporphyrin thin-film transistors J. 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Downloaded to IP: 141.223.173.110 On: Tue, 21 Apr 2015 07:14:39 APPLIED PHYSICS LETTERS 87, 152105 共2005兲 Influence of the dielectric constant of a polyvinyl phenol insulator on the field-effect mobility of a pentacene-based thin-film transistor Yunseok Jang, Do Hwan Kim, Yeong Don Park, Jeong Ho Cho, Minkyu Hwang, and Kilwon Choa兲 Department of Chemical Engineering, Pohang University of Science and Technology, Pohang 790-784, Korea 共Received 1 June 2005; accepted 31 August 2005; published online 5 October 2005兲 The mobility of pentacene thin-film transistors 共TFTs兲 is correlated with the dielectric properties of their insulators. We varied the dielectric properties of the poly共4-vinylphenol兲 insulators of such TFTs by changing the molar ratio of the prepolymer/cross-linking agent while keeping the surface potential of the insulator surface constant. It was found that the field-effect mobility of the pentacene TFTs increases with increases in the dielectric constant of the insulators. A small increase in the dielectric constant of the insulator 共a 20% increase, 3.6–4.3兲 was found to result in a dramatic increase in the field-effect mobility of pentacene TFTs by a factor of 3 共0.26 to 0.81 cm2 / V s兲. © 2005 American Institute of Physics. 关DOI: 10.1063/1.2093940兴 The insulator is a crucial component of organic fieldeffect transistors 共OTFTs兲. This is especially true in the case of “bottom gate” architectures in which the semiconductor is deposited on top of the insulator and the surface characteristics of the insulator strongly influence the quality of the insulator-semiconductor interface, significantly affecting the performance of the device. In the last decade, a considerable number of studies have been devoted to the fabrication of OFETs 共Refs. 1–6兲 using organic insulators7–13 for use as switching devices for flexible displays. However, although great advances have been made in the improvement of OFETs using polymer insulators, there has been relatively little research into the effects of the dielectric properties of polymer insulators on device performance.13–15 Peng et al. showed a correlation between the device field-effect mobility and the dielectric constant of the insulator.14 However, the relationship between the dielectric constant of the insulator and the electric properties of the device was not sufficiently clear in their system, because they used different types of polymer insulators with different surface potentials. In the case of semicrystalline organic semiconductors such as pentacene, the morphology and molecular ordering of the semiconductor at the insulator-semiconductor interface have a significant influence on the field-effect mobility of the device, and is determined by the quality of the insulatorsemiconductor interface, especially by the surface potential of the insulator.4,16–20 In their study, the effects of surface potential and those of the dielectric properties of the insulator were not distinguished. In the present study, in order to investigate the effects of varying the dielectric constant of the insulator on the electric properties of FETs, we used only one kind of polymer insulator, polyvinyl phenol 共PVP兲, and varied the molar ratio of prepolymer and cross-linking agent, thus changing only the dielectric constant while keeping the surface energy of the polymer insulator constant. The M w of the polyvinyl phenol prepolymer was ⬇20 kg/ mol. We used poly共melamine-co-formaldehyde兲 a兲 Author to whom correspondence should be addressed; electronic mail: kwcho@postech.ac.kr 关PMF兴 as the cross-linking agent. PVP and PMF were dissolved in propylene glycol methyl ether acetate 关PGMEA兴 共about 13– 15 wt. %兲 with mole ratios of 20:1, 5:1, 7:1, and 1:1. The insulator films were formed by spin coating the prepared solutions at 3000 rpm on heavily doped n-type Si wafers as gate electrodes, with subsequent cross-linking for 1 h at 200 ° C in a vacuum oven. The rms roughnesses measured with AFM and the surface energies of the polymer insulators are shown in Table I. The surface energies of the insulators were determined from contact angle measurements using distilled water and diiodomethane as a probe liquid and the geometric mean equation,21 共1 + cos 兲␥ pl = 2共␥sd␥dpl兲1/2 + 2共␥sp␥ ppl兲1/2 , where ␥s and ␥ pl are the surface energies of the sample and the probe liquid, respectively, and the superscripts d and p refer to the dispersion and polar 共nondispersion兲 components of the surface energy, respectively. As can be seen in Table I, the prepared polymer insulators have similar rms roughnesses, 0.3– 0.4 nm, and surface energies, ⬇42 mJ/ m2. Table I shows the dielectric constants k of the polymer insulators, as obtained with the following equation:22 k= Ct , A0 where C is the capacitance of the insulator, A is the dot area 共0.005 cm2兲, t is the insulator thickness 共⬃350 nm兲, and 0 is the permittivity in vacuum 共8.85⫻ 10−14 F cm−1兲. The capacitance, C, was obtained from C-V measurements 共Agilent 4284A兲 and the thicknesses of the polymer insulators were measured with ellipsometry. Table I shows that the dielectric constant decreases with increases in cross-linking density and varies from 3.6 to 4.3 with increases in the molar ratio. The dielectric constant reveals significant information about the chemical and physical state of a polymer, since it is drastically affected by the presence of another polymer or a dopant.23,24 Therefore the variation of the dielectric constant with molar ratio is caused by the presence of another polymer 共the cross-linking agent兲 in PVP and the number of hydroxyl groups of PVP in the insu- This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: 0003-6951/2005/87共15兲/152105/3/$22.50 87, 152105-1 © 2005 American Institute of Physics 141.223.173.110 On: Tue, 21 Apr 2015 07:14:39 152105-2 Appl. Phys. Lett. 87, 152105 共2005兲 Jang et al. TABLE I. Properties of pentacene devices with PVP insulators prepared with various PVP/PMF ratios. Insulator Device Field-effect On/off Threshold Equivalent Surface rms ratio roughness energy Dielectric mobility current voltage ratio 共V兲 共PVP:PMF兲 共Å兲 共mJ/ m2兲 constant 共cm2 / V s兲 20:1 5:1 1.7:1 1:1 3 3 4 4 42.5 42.6 42.3 42.2 4.3共±0.1兲 4.1共±0.1兲 3.8共±0.1兲 3.6共±0.1兲 0.81 0.62 0.34 0.26 3.5⫻ 103 8.5⫻ 102 1.9⫻ 104 8.1⫻ 103 −14.6 −15.9 −20.3 −21.5 lator. Thus we were able to successfully vary the dielectric constant of the polymer insulator in the range 3.6–4.3 while keeping the surface potential of the insulator constant. The 26 nm pentacene film was deposited on top of the insulator surface at a deposition rate of 0.4 Å s−1 at 70 ° C by using the thermal evaporation method. Figure 1 shows AFM images of the pentacene films deposited on the polymer insulators prepared with different 共PVP:PMF兲 ratios. The surface morphologies and grain sizes of the pentacene films on the polymer insulators are very similar 共⬃200 nm in diameter兲. This result indicates that the pentacene crystal grain size is not an important parameter in our system. Figure 1 shows the reflective x-ray diffraction patterns of pentacene films grown on polymer insulators prepared with various 共PVP:PMF兲 ratios. The typical x-ray diffraction pattern of pentacene includes two distinct crystalline phases, the “thin-film phase” and the “single-crystal phase,” with correand 14.5 Å, sponding d001-spacings of 15.4 Å respectively.25,26 All samples produced sharp first-order diffraction peaks at 5.72° corresponding to a lattice spacing of 15.4 Å, which indicates the presence of only a single “thinfilm phase.” The diffraction results also clearly demonstrate that the ordering of the pentacene molecules grown on the four different polymer insulators with different 共PVP:PMF兲 ratios is the same. This result is expected from the results for the surface energies and rms roughnesses of the insulator surfaces, and is consistent with the results for the surface morphologies. FIG. 2. The drain current 共ID兲 vs drain voltage 共VD兲 characteristics of a pentacene TFT prepared with a PVP:PMF ratio of 1:1. A top-contact thin film transistor 共TFT兲 with a gold electrode 共channel width 800 m, length 40 m兲 was used for analyzing the electrical characteristics of the pentacene TFTs. Current-voltage measurements were carried out in air at room temperature using Keithley 236 voltage source units. Figure 2 shows the drain current 共ID兲 vs drain voltage 共VD兲 curve obtained for the OTFT fabricated with a PVP:PMF ratio of 1:1. This figure shows a typical output characteristic of transistors. In Fig. 3, the square root of 兩ID兩 in the saturation region at VD = −40 V is plotted as a function of gate voltage VG for the prepared devices. From each linear fit in Fig. 3, the threshold voltage Vth and field-effect mobility in the saturation region were determined with the following equation:27 兩ID兩 = W C共VG − Vth兲2 , 2L where C is the capacitance of the polymer insulator, W is the channel width, L is the channel length, Vth is the threshold voltage, and is the field-effect mobility. The characteristic electric properties of the four devices are summarized in Table I. Field-effect mobilities of 0.26– 0.81 cm2 / V s and threshold voltages of −14.5 to − 21.5 V were obtained. The field-effect mobility increases and the absolute value of the threshold voltage decreases with increases in the dielectric constant of the insulator. This result agrees with previous results.14,15 Surprisingly, the field-effect mobility increases by a factor of approximately 3 with only a small change 共3.6–4.3, a 20% increase兲 in the dielectric constant, k, of the insulator. The higher field-effect mobility for insulators with higher dielectric constants may be due to their enhanced polarization, which increases the number of hole-carriers at the insulator-semiconductor interface. As a result, for the same gate field, a higher mobility is obtained for devices with higher k insulators.28,29 In summary, we have varied the dielectric constant of a PVP insulator by varying the polymer/cross-linking agent molar ratio while keeping other parameters such as the roughness and surface potential of the insulator constant; these insulators with different dielectric constants produce similar film morphologies and molecular ordering. The fieldeffect mobility was found to increase by a factor of more FIG. 1. 共a兲 X-ray diffraction patterns of pentacene films grown on insulathan 3 with small changes 共less than 20%兲 in the dielectric tors; 共b兲 AFM micrographs of pentacene on insulators prepared with various This article is copyrighted as indicated in the article. Reuse of AIP content is subject to the terms at: http://scitation.aip.org/termsconditions. Downloaded to IP: constant of the insulator. 共PVP/PMF兲 ratios: 20:1, 5:1, 1.7:1, 1:1. 141.223.173.110 On: Tue, 21 Apr 2015 07:14:39 152105-3 Appl. Phys. Lett. 87, 152105 共2005兲 Jang et al. FIG. 3. 冑兩ID兩 vs VG and log10兩ID兩 vs VG characteristics of pentacene TFTs prepared with various 共PVP:PMF兲 ratios: 共a兲 20:1, 共b兲 5:1, 共c兲 1.7:1, 共d兲 1:1 This work was supported by the National Research Laboratory Program of the Ministry of Science and Technology of Korea, a grant 共F0004022兲 from the Information Display R&D Center under the 21st Century Frontier R&D Program and the Regional R&D Cluster Project designated by the Ministry of Commerce, Industry and Energy of Korea, and the BK21 Program of the Ministry of Education and Human Resources Development of Korea. We also thank the Pohang Acceleratoty Laboratory for providing the synchrotron radiation source at the 3C2 and 8C1 beam line. C. H. Dimitrakopoulos and P. R. L. Malenfant, Adv. Mater. 共Weinheim, Germany兲 14, 99 共2002兲. 2 G. 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