Browsing by Author "Liu, Chih-Ming"

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A nanostructured micellar diblock copolymer layer affects the memory characteristics and packing of pentacene molecules in non-volatile organic field-effect transistor memory devices
(2013)
Chen, Chia-Min
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Liu, Chih-Ming
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Tsai, Ming-Chang
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Chen, Hsiu-Cheng
;
Wei, Kung-Hwa
Organic field-effect transistor (OFET) memory devices incorporating the copolymer polystyrene-block-poly(4-vinylpyridine) (PS56k-b-P4VP(8k)) layer, which features a thickness-dependent micellar nanostructure (P4VP-core, PS-shell), as a charge trapping layer can exhibit tunable memory windows for p-channel applications. For instance, the memory window increased substantially from 7.8 V for the device incorporating a 60 nm thick PS56k-b-P4VP(8k) layer to 21 V for the device incorporating a 27 nm thick layer, an increase of more than 2.5 times. Using simultaneous synchrotron grazing-incidence small-angle X-ray scattering and wide-angle X-ray scattering to probe the nanostructured micellar PS56k-b-P4VP(8k) layer and the pentacene layer positioned directly on the top of the copolymer layers, respectively, we were able to elucidate the structural characteristics of the bilayer and to correlate their effects with the memory performances of devices with similar architectures. For the PS56k-b-P4VP(8k) layers, we found that the inter-micelle distance and their lateral arrangements depended on the layer thickness: the thickness of the PS shells in the lateral direction decreased upon increasing the layer thickness, as did the memory window for the OFET device that incorporated the PS56k-b-P4VP(8k) layers, showing a strong dependence of the threshold voltage shifts (i.e., memory window) on the distance between the micelles. Additionally, for the molecular packing of the pentacene layer positioned on the copolymer layer, we found that the PS56k-b-P4VP(8k) layers affected not only the orientation of the pentacene molecules but also their grain sizes, thereby affecting the hole mobility of the memory devices. These results suggest that tuning the micellar nanostructure of the block copolymer thin film that was used as a trapping layer can be a simple and effective way for optimizing the memory window and affecting the hole mobility of OFET memory devices.
Complementary solvent additives tune the orientation of polymer lamellae, reduce the sizes of aggregated fullerene domains, and enhance the performance of bulk heterojunction solar cells
(2014-01-01)
Liu, Chih-Ming
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Su, Yu-Wei
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Jiang, Jian-Ming
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Chen, Hsiu-Cheng
;
Lin, Shu-Wei
In this study we employed 1-chloronaphthalene (CN) and 1,8-diiodooctane (DIO) as binary additives exhibiting complementarily preferential solubility for processing the crystalline conjugated polymer poly[bis(dodecyl)thiophene-dodecyl-thieno[3,4-c]pyrrole-4,6-dione] (PBTC12TPD) and the fullerene [6,6]-phenyl-C-71-butyric acid methyl ester (PC71BM) in chloroform. Using synchrotron grazing-incidence small-/wide-angle X-ray scattering and transmission electron microscopy to analyse the structure of the PBTC12TPD-PC71BM blend films, we found that the binary additives with different volume ratios in the processing solvent allow us to tune the relative population of face-on to edge-on PBTC12TPD lamellae and the size of PC71BM clusters in the blend films; the sizes of the fractal-like PC71BM clusters and the aggregated domains of PC71BM clusters increased and decreased, respectively, upon increasing the amount of DIO, whereas the relative ratio of face-on to edge-on PBTC12TPD lamellae increased upon increasing the amount of CN. When fabricating the photovoltaic devices, the short-circuit current density of the devices with the PBTC12TPD-PC71BM active layer having been processed with the binary additives is higher than that of the device incorporating an active layer processed without any additive. As a result, the power conversion efficiency of a device incorporating an active layer of PBTC12TPD-PC71BM (1 : 1.5, w/w) processed with binary additives of 0.5% DIO and 1% CN in chloroform increased to 6.8% from a value of 4.9%, a relative increase of 40%, for the corresponding device containing the same active layer but processed without any additive.
Distribution of Crystalline Polymer and Fullerene Clusters in Both Horizontal and Vertical Directions of High-Efficiency Bulk Heterojunction Solar Cells
(2013-06-26)
Liu, Chih-Ming
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Su, Ming-Shin
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Jiang, Jian-Ming
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Su, Yu-Wei
;
Su, Chun-Jen
In this study, we used (i) synchrotron grazing-incidence small-/wide-angle X-ray scattering to elucidate the crystallinity of the polymer PBTC12TPD and the sizes of the clusters of the fullerenes PC61BM and ThC61BM and (ii) transmission electron microscopy/electron energy loss spectroscopy to decipher both horizontal and vertical distributions of fullerenes in PBTC12TPD/fullerene films processed with chloroform, chlorobenzene and dichlorobezene. We found that the crystallinity of the polymer and the sizes along with the distributions of the fullerene clusters were critically dependent on the solubility of the polymer in the processing solvent when the solubility of fullerenes is much higher than that of the polymer in the solvent. In particular, with chloroform (CF) as the processing solvent, the polymer and fullerene units in the PBTC12TPD/ThC61BM layer not only give rise to higher crystallinity and a more uniform and finer fullerene cluster dispersion but also formed nanometer scale interpenetrating network structures and presented a gradient in the distribution of the fullerene clusters and polymer, with a higher polymer density near the anode and a higher fullerene density near the cathode. As a result of combined contributions from the enhanced polymer crystallinity, finer and more uniform fullerene dispersion and gradient distributions, both the short current density and the fill factor for the device incorporating the CF-processed active layer increase substantially over that of the device incorporating a dichlorobenzene-processed active layer; the resulting power conversion efficiency of the device incorporating the CF-processed active layer was enhanced by 46% relative to that of the device incorporating a dichlorobenzene-processed active layer.
Effects of bulk and interfacial charge accumulation on fill factor in organic solar cells
(2013-05-13)
Chen, Bingbing
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Qiao, Xianfeng
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Liu, Chih-Ming
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Zhao, Chen
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Chen, Hsiu-Cheng
The effects of charge accumulation on fill factor (FF) are studied by using light intensity-dependent current-voltage and capacitance-voltage measurements based on poly-{bi(dodecyl) thiophene-thieno[ 3,4-c]pyrrole-4,6-dione}:1(3-methyloxycarbonyl)propyl-1-phenyl [6,6] (PBTTPD:PCBM) solar cells. We find that the FF of un-annealed device shows a non-monotonic dependence of light intensity: first an increase and then a decrease with increasing light intensity. This suggests that both bulk charge accumulation and recombination determine the FF before thermal annealing. Furthermore, the morphological enhancement of PBTTPD: PCBM film leads to a monotonic decrease of FF as increasing light intensity. This indicates that only surface charge accumulation plays an important role in the determination of the FF after thermal annealing. (C) 2013 AIP Publishing LLC.
Non-volatile organic field-effect transistor memory comprising sequestered metal nanoparticles in a diblock copolymer film
(2012-01-14)
Chen, Chia-Min
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Liu, Chih-Ming
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Wei, Kung-Hwa
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Jeng, U-Ser
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Su, Chiu-Hun
In this study, we fabricated p-channel-type non-volatile organic field-effect transistor (OFET) memory devices featuring an asymmetric PS-b-P4VP diblock copolymer layer incorporating high- and low-work-function metal nanoparticles (NPs) in the hydrophilic and hydrophobic blocks, respectively. We chose the highly asymmetric diblock copolymer PS(56k)-b-P4VP(8k) as the polymer electret to create the memory windows, and used the different work functions of the ex situ-synthesized metal NPs to tune the memory window for either p- or n-channel applications. The transfer curves of non-volatile OFET memory devices incorporating an asymmetric PS(56k)-b-P4VP8k layer embedded with high-work-function Pt NPs (5.65 eV) in the P4VP block exhibited a positive threshold voltage shift and a large memory window (ca. 27 V). In contrast, the transfer curves of the corresponding non-volatile OFET memory devices featuring embedded low-work-function (4.26 eV) Ag NPs exhibited a negative threshold voltage shift and a smaller memory window (ca. 19 V). This approach provides a versatile way to fabricate p- or possibly n-channel-type non-volatile organic field-effect transistor (OFET) memory devices with the same processing procedure.
Structural Evolution of Crystalline Conjugated Polymer/Fullerene Domains from Solution to the Solid State in the Presence and Absence of an Additive
(2015-02-12)
Su, Yu-Wei
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Liu, Chih-Ming
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Jiang, Jian-Ming
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Tsao, Cheng-Si
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Cha, Hou-Chin
The power conversion efficiencies of polymer/fullerene solar cells are critically dependent on the nanometer-scale morphologies of their active layers, which are typically processed from solution. Using synchrotron wide- and small-angle X-ray scattering, we have elucidated the intricate mechanism of the structural transitions from solutions to solid films of the crystalline polymer poly[bis(dodecyl)thiophene-thieno[3,4-c]pyrrole-4,6-dione] (PBTTPD) and [6,6]-phenyl-C-71-butyric acid methyl ester (PC71BM), including the effect of the solvent additive 1,6-diiodohexane (DIH). We found that the local assembly of rigid-rod PBTTPD segments that formed in solution instantly and then relaxed within several hundred seconds upon cooling to room temperature from 90 degrees C could re-emerge and develop into seeds for subsequent crystallization of the polymer in the solid films. At room temperature (25 degrees C), the presence of DIH in chlorobenzene slightly enhanced the formation of local assembly PBTTPD segments in the supersaturated PBTTPD in PBTTPD/PC71BM blend solution. Two cases of films were subsequently developed from these blend solutions with drop-casted and spin-coated methods. For spin-coated thin films (90 nm thick), which evolve quickly, polymers crystallinity and the fullerene packing in the solid-state thin films were enhanced in the case of involving DIH. Regarding the effect of DIH for processing the drop-casted thick films (2.5 mu m thick), which evolve slowly, DIH has no observable effect on PBTTPD/PC71BM structure. Our results provide some understanding of the mechanism behind the structural development of polymer/fullerene blends upon their transitions from solution to the solid state, as well as the key functions of the additive.
Surface Layering and Supersaturation for Top-Down Nanostructural Development during Spin Coating of Polymer/Fullerene Thin Films
(2017-07-19)
Wu, Wei-Ru
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Su, Chun-Jen
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Chuang, Wei-Tsung
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Huang, Yen-Chih
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Yang, Po-Wei
This study provides new evidence on a long postulated mechanism of phase separation in a polymer/fullerene mixture during spin coating for controlled nanodomains of oriented crystallization and heterojunctions that favor applications in polymer solar cells (PSCs). The simultaneous nanoscale phase separation and crystallization during spin coating of the mixture are traced using in situ grazing-incidence small-and wide-angle X-ray scattering. Combined with the complimentary results from time-resolved optical reflectance spectroscopy, transient stratification of the liquid film during the transition from the flow-to evaporation-dominated stage of spin coating is disclosed; the vertical liquid-liquid phase separation incubates a supersaturated skin layer where fullerene aggregation and polymer crystallization occur and develop concomitantly. Shortly after the transition, the near-surface structural development is largely pinned, leaving the solvent-rich bottom layer to diminish via solvent diffusion and evaporation through the thickened skin layer that finally condenses into the spin-coated film upon solvent depletion. The shear-enhanced surface layering and supersaturation for the surface-down nanostructural development are unexpected in all the existing structural models for PSCs. The mechanistic understanding of coupled vertical phase separation and local nanosegregation provides new insights and alternative strategy to the morphology control of spin-cast PSC active layers in particular and various solution-processed polymeric films in general.
Symmetry and Coplanarity of Organic Molecules Affect their Packing and Photovoltaic Properties in Solution-Processed Solar Cells
(2014-06-25)
Lan, Shang-Che
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Raghunath, Putikam
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Lu, Yueh-Hsin
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Wang, Yi-Chien
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Lin, Shu-Wei
In this study we synthesized three acceptor donor acceptor (A-D-A) organic molecules, TB3t-BT, TB3t-BTT, and TB3t-BDT, comprising 2,2\'-bithiophene (BT), benzo[1,2-b:3,4-b\':5,6-d \'\']trithiophene (BTT), and benzo[ 1,2-b;4,5-b\']dithiophene (BDT) units, respectively, as central cores (donors), terthiophene (3t) as pi-conjugated spacers, and thiobarbituric acid (TB) units as acceptors. These molecules display different degrees of coplanarity as evidenced by the differences in dihedral angles calculated from density functional theory. By using differential scanning calorimetry and X-ray diffractions for probing their crystallization characteristics and molecular packing in active layers, we found that the symmetry and coplanarity of molecules would significantly affect the melting/crystallization behavior and the formation of crystalline domains in the blend film with fullerene, PC61BM. TB3t-BT and TB3t-BDT, which each possess an inversion center and display high crystallinity in their pristine state, but they have different driving forces in crystallization, presumably because of different degrees of coplanarity. On the other hand, the asymmetrical TB3t-BTT behaved as an amorphous material even though it possesses a coplanar structure. Among our tested systems, the device comprising as-spun TB3t-BDT/PC61BM (6:4, w/w) active layer featured crystalline domains and displayed the highest power conversion efficiency (PCE) of 4.1%. In contrast, the as-spun TB3t-BT/PC61BM (6:4, w/w) active layer showed well-mixed morphology and with a device PCE of 0.2%; it increased to 3.9% after annealing the active layer at 150 degrees C for 15 min. As for TB3t-BTT, it required a higher content of fullerene in the TB3t-BTT/PC61BM (4:6, w/w) active layer to optimize its device PCE to 1.6%.
The dual localized surface plasmonic effects of gold nanodots and gold nanoparticles enhance the performance of bulk heterojunction polymer solar cells
(2013-10-01)
Liu, Chih-Ming
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Chen, Chia-Min
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Su, Yu-Wei
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Wang, Shu-Min
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Wei, Kung-Hwa
In this study, we investigated the effects of plasmonic resonances induced by gold nanodots (Au NDs), thermally deposited on the active layer, and octahedral gold nanoparticles (Au NPs), incorporated within the hole transport layer, on the performance of bulk heterojunction polymer solar cells (PSCs) based on poly(3-hexyl thiophene) (P3HT) and [ 6,6]-phenyl-C(61)butyric acid methyl ester (PC61BM). Thermal deposition of 5.3-nm Au NDs between the active layer and the cathode in a P3HT:PC61BM device resulted in the power conversion efficiency (PCE) of 4.6%-that is 15% greater than that (4.0%) for the P3HT:PC61BM device without Au NDs. The Au NDs provided near-field enhancement through excitation of the localized surface plasmon resonance (LSPR), thereby enhancing the degree of light absorption. In addition to the thermally deposited Au-NDs, embedding Au NPs within the poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) to form a dual metallic nanostructure can further enhance PCE to 4.8%-that is about 20% greater than that of the conventional P3HT:PC61BM cell. Thus, Au NPs and Au NDs appear to have great potential for the application in high-efficiency LSPR-enhanced PSCs. (C) 2013 Published by Elsevier B.V.