Surface-enhanced Raman spectroscopic studies of the Au-pentacene interface: a combined experimental and theoretical investigation.

PubMed

Adil, D; Guha, S

2013-07-28

It has recently been shown [D. Adil and S. Guha, J. Phys. Chem. C 116, 12779 (2012)] that a large enhancement in the Raman intensity due to surface-enhanced Raman scattering (SERS) is observed from pentacene when probed through the Au contact in organic field-effect transistors (OFET) structures. Here, the SERS spectrum is shown to exhibit a high sensitivity to disorder introduced in the pentacene film by Au atoms. The Raman signature of the metal-semiconductor interface in pentacene OFETs is calculated with density-functional theory by explicitly considering the Au-pentacene interaction. The observed enhancement in the 1380 cm(-1) and the 1560 cm(-1) regions of the experimental Raman spectrum of pentacene is successfully modeled by Au-pentacene complexes, giving insights into the nature of disorder in the pentacene sp(2) network. Finally, we extend our previous work on high-operating voltage pentacene OFETs to low-operating voltage pentacene OFETs. No changes in the SERS spectra before and after subjecting the OFETs to a bias stress are observed, concurrent with no degradation in the threshold voltage. This shows that bias stress induced performance degradation is, in part, caused by field-induced structural changes in the pentacene molecule. Thus, we confirm that the SERS spectrum can be used as a visualization tool for correlating transport properties to structural changes, if any, in organic semiconductor based devices.

Firefly

DTIC Science & Technology

2012-05-29

Hunter College has completed work on baseline measurements of relaxation times for pentacene at various temperatures in order to determine optimal...temperatures for measuring relaxation rate as a function of doping. We have also repeated these measurements on pentacene samples at 2 different...P3HT using a time-lag method. 2 Technical Accomplishments This Period Relaxation Measurements on Pentacene . As described initially in the 1Q

Epitaxial growth of pentacene on alkali halide surfaces studied by Kelvin probe force microscopy.

PubMed

Neff, Julia L; Milde, Peter; León, Carmen Pérez; Kundrat, Matthew D; Eng, Lukas M; Jacob, Christoph R; Hoffmann-Vogel, Regina

2014-04-22

In the field of molecular electronics, thin films of molecules adsorbed on insulating surfaces are used as the functional building blocks of electronic devices. Control of the structural and electronic properties of the thin films is required for reliably operating devices. Here, noncontact atomic force and Kelvin probe force microscopies have been used to investigate the growth and electrostatic landscape of pentacene on KBr(001) and KCl(001) surfaces. We have found that, together with molecular islands of upright standing pentacene, a new phase of tilted molecules appears near step edges on KBr. Local contact potential differences (LCPD) have been studied with both Kelvin experiments and density functional theory calculations. Our images reveal that differently oriented molecules display different LCPD and that their value is independent of the number of molecular layers. These results point to the formation of an interface dipole, which may be explained by a partial charge transfer from the pentacene to the surface. Moreover, the monitoring of the evolution of the pentacene islands shows that they are strongly affected by dewetting: Multilayers build up at the expense of monolayers, and in the Kelvin images, previously unknown line defects appear, which reveal the epitaxial growth of pentacene crystals.

Characterization and Modeling of Nano-organic Thin Film Phototransistors Based on 6,13(Triisopropylsilylethynyl)-Pentacene: Photovoltaic Effect

NASA Astrophysics Data System (ADS)

Jouili, A.; Mansouri, S.; Al-Ghamdi, Ahmed A.; El Mir, L.; Farooq, W. A.; Yakuphanoglu, F.

2017-04-01

Organic thin film transistors based on 6,13(triisopropylsilylethynyl)-pentacene (TIPS-pentacene) with various channel widths and thicknesses of the active layer (300 nm and 135 nm) were photo-characterized. The photoresponse behavior and the gate field dependence of the charge transport were analyzed in detail. The surface properties of TIPS-pentacene deposited on silicon dioxide substrate were investigated using an atomic force microscope. We confirm that the threshold voltage values of the TIPS-pentacene transistor depend on the intensity of white light illumination. With the multiple trapping and release model, we have developed an analytical model that was applied to reproduce the experimental output characteristics of organic thin film transistors based on TIPS-pentacene under dark and under light illumination.

Symmetry lowering of pentacene molecular states interacting with a Cu surface

NASA Astrophysics Data System (ADS)

Baldacchini, Chiara; Mariani, Carlo; Betti, Maria Grazia; Vobornik, Ivana; Fujii, Jun; Annese, Emilia; Rossi, Giorgio; Ferretti, Andrea; Calzolari, Arrigo; di Felice, Rosa; Ruini, Alice; Molinari, Elisa

2007-12-01

Pentacene adsorbed on the Cu(119) vicinal surface forms long-range ordered chain structures. Photoemission spectroscopy measurements and ab initio density functional theory simulations provide consistent evidences that pentacene molecular orbitals mix with the copper bands, giving rise to interaction states localized at the interface. Angular-resolved and polarization dependent photoemission spectroscopy shows that most of the pentacene derived intensity is strongly dichroic. The symmetry of the molecular states of the free pentacene molecules is reduced upon adsorption on Cu(119), as a consequence of the molecule-metal interaction. Theoretical results show a redistribution of the charge density in π molecular states close to the Fermi level, consistent with the photoemission intensities (density of states) and polarization dependence (orbital symmetry).

Structure and properties of small molecule-polymer blend semiconductors for organic thin film transistors.

PubMed

Kang, Jihoon; Shin, Nayool; Jang, Do Young; Prabhu, Vivek M; Yoon, Do Y

2008-09-17

A comprehensive structural and electrical characterization of solution-processed blend films of 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS-pentacene) semiconductor and poly(alpha-methylstyrene) (PalphaMS) insulator was performed to understand and optimize the blend semiconductor films, which are very attractive as the active layer in solution-processed organic thin-film transistors (OTFTs). Our study, based on careful measurements of specular neutron reflectivity and grazing-incidence X-ray diffraction, showed that the blends with a low molecular-mass PalphaMS exhibited a strong segregation of TIPS-pentacene only at the air interface, but surprisingly the blends with a high molecular-mass PalphaMS showed a strong segregation of TIPS-pentacene at both air and bottom substrate interfaces with high crystallinity and desired orientation. This finding led to the preparation of a TIPS-pentacene/PalphaMS blend active layer with superior performance characteristics (field-effect mobility, on/off ratio, and threshold voltage) over those of neat TIPS-pentacene, as well as the solution-processability of technologically attractive bottom-gate/bottom-contact OTFT devices.

Triplet exciton dissociation and electron extraction in graphene-templated pentacene observed with ultrafast spectroscopy.

PubMed

McDonough, Thomas J; Zhang, Lushuai; Roy, Susmit Singha; Kearns, Nicholas M; Arnold, Michael S; Zanni, Martin T; Andrew, Trisha L

2017-02-08

We compare the ultrafast dynamics of singlet fission and charge generation in pentacene films grown on glass and graphene. Pentacene grown on graphene is interesting because it forms large crystals with the long axis of the molecules "lying-down" (parallel to the surface). At low excitation fluence, spectra for pentacene on graphene contain triplet absorptions at 507 and 545 nm and no bleaching at 630 nm, which we show is due to the orientation of the pentacene molecules. We perform the first transient absorption anisotropy measurements on pentacene, observing negative anisotropy of the 507 and 545 nm peaks, consistent with triplet absorption. A broad feature at 853 nm, observed on both glass and graphene, is isotropic, suggesting hole absorption. At high fluence, there are additional features, whose kinetics and anisotropies are not explained by heating, that we assign to charge generation; we propose a polaron pair absorption at 614 nm. The lifetimes are shorter at high fluence for both pentacene on glass and graphene, indicative of triplet-triplet annihilation that likely enhances charge generation. The anisotropy decays more slowly for pentacene on graphene than on glass, in keeping with the smaller domain size observed via atomic force microscopy. Coherent acoustic phonons are observed for pentacene on graphene, which is a consequence of more homogeneous domains. Measuring the ultrafast dynamics of pentacene as a function of molecular orientation, fluence, and polarization provides new insight to previous spectral assignments.

Meso-size Effect from Self-assembled Carbon Structures and Their Device Applications

DTIC Science & Technology

2013-08-23

electrical photoresponse from pentacene 1D disks and 2D wires, and 3) dramatic increase of solubility in water of zinc phthalocyanine (ZnPc) nanowires...Hong, M.; Son, M.; Choi, H. C.* “Crystal Plane-Dependent Photoluminescence Activity of Pentacene 1D Wire and 2D Disk Crystals.” Angew. Chem. Int...Ed. 2013, 52, 5997-6001. [7] Park, J. E.; Hong, M.; Son, M.; Choi, H. C.* “Crystal Plane-Dependent Photoluminescence Activity of Pentacene 1D Wire

Photon Antibunching in the Fluorescence of a Single Dye Molecule Trapped in a Solid

DTIC Science & Technology

1992-06-08

number) FIELD GROUP SUB-GROUP single-molecule spectroscopy in solids, photon antibunching, quantum-optics, nonclassical effects pentacene in p-terphenyl...emitted by an optically pumped single molecule of pentacene In a p-terphenyl host has been Investigated at short times. The correlation function...excitation tcclnique, certain individual pentacene impurity molecules in a p-terphenyl crystal 11 were observed to spectrally diffuse, i.e. their absorption

Tuning pentacene based dye-sensitized solar cells.

PubMed

Kunzmann, Andreas; Gruber, Marco; Casillas, Rubén; Tykwinski, Rik R; Costa, Rubén D; Guldi, Dirk M

2018-05-10

We report on the synthesis, as well as photophysical and electrochemical characterization of a new family of pentacene derivatives, which are applied in n-type dye-sensitized solar cells (DSSCs). As far as the molecular structure of the pentacene is concerned, the synthetic design focuses on cyano acrylic tethered at the 13-position of the pentacene chromophore. The electrolyte composition features increasing amounts of Li+ ions as an additive. In general, the increase of Li+ concentrations extrinsically reduces the quasi Fermi level of the photoanode and as such facilitates the electron injection process. We demonstrate that pentacene derivatives give rise to a unique charge injection process, which is controlled by the positioning of the quasi Fermi level energies as a function of the Li+ concentration. As a result of the enhanced charge injection, device efficiencies as high as 1.5% are achieved, representing a 3-fold increase from previously reported efficiencies in pentacene-based DSSCs. These findings are supported by device analysis in combination with transient absorption and electrochemical impedance spectroscopy assays.

Enhanced Performance Consistency in Nanoparticle/TIPS Pentacene-Based Organic Thin Film Transistors

DOE Office of Scientific and Technical Information (OSTI.GOV)

He, Zhengran; Xiao, Kai; Durant, William Mark

2011-01-01

In this study, inorganic silica nanoparticles are used to manipulate the morphology of 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS pentacene) thin films and the performance of solution-processed organic thin-film transistors (OTFTs). This approach is taken to control crystal anisotropy, which is the origin of poor consistency in TIPS pentacene based OTFT devices. Thin film active layers are produced by drop-casting mixtures of SiO{sub 2} nanoparticles and TIPS pentacene. The resultant drop-cast films yield improved morphological uniformity at {approx}10% SiO{sub 2} loading, which also leads to a 3-fold increase in average mobility and nearly 4 times reduction in the ratio of measured mobility standard deviationmore » ({mu}{sub Stdev}) to average mobility ({mu}{sub Avg}). Grazing-incidence X-ray diffraction, scanning and transmission electron microscopy as well as polarized optical microscopy are used to investigate the nanoparticle-mediated TIPS pentacene crystallization. The experimental results suggest that the SiO{sub 2} nanoparticles mostly aggregate at TIPS pentacene grain boundaries, and 10% nanoparticle concentration effectively reduces the undesirable crystal misorientation without considerably compromising TIPS pentacene crystallinity.« less

Variable charge transfer state energies at nanostructured pentacene/C60 interfaces

NASA Astrophysics Data System (ADS)

Lin, YunHui L.; Zhang, Fengyu; Kerner, Ross A.; Yang, Terry Chien-Jen; Kahn, Antoine; Rand, Barry P.

2018-05-01

While it has recently been recognized that organic donor-acceptor charge transfer (CT) state energies can vary substantially under different interfacial morphologies, this behavior is under-appreciated in the context of organic singlet fission solar cells where a specific alignment between the triplet state of the fission material and the CT state of the donor-acceptor interface is necessary to the function of the device. In this work, we demonstrate that the CT state energy of a prototypical pentacene-C60 singlet fission system is around 1 eV in most systems, but can vary over 300 meV depending on the composition and morphology of the interface. Moreover, we show that the inclusion of a poly(3-hexylthiophene-2,5-diyl) underlayer, which commonly serves as a triplet blocker and hole collector in pentacene/C60 solar cells, helps promote active layer morphologies with stabilized, low energy CT states. These trends in the interfacial energetics are correlated with structural characterization of the films by atomic force microscopy and x-ray diffraction.

Thin-film morphology of inkjet-printed single-droplet organic transistors using polarized Raman spectroscopy: effect of blending TIPS-pentacene with insulating polymer.

PubMed

James, David T; Kjellander, B K Charlotte; Smaal, Wiljan T T; Gelinck, Gerwin H; Combe, Craig; McCulloch, Iain; Wilson, Richard; Burroughes, Jeremy H; Bradley, Donal D C; Kim, Ji-Seon

2011-12-27

We report thin-film morphology studies of inkjet-printed single-droplet organic thin-film transistors (OTFTs) using angle-dependent polarized Raman spectroscopy. We show this to be an effective technique to determine the degree of molecular order as well as to spatially resolve the orientation of the conjugated backbones of the 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-Pentacene) molecules. The addition of an insulating polymer, polystyrene (PS), does not disrupt the π-π stacking of the TIPS-Pentacene molecules. Blending in fact improves the uniformity of the molecular morphology and the active layer coverage within the device and reduces the variation in molecular orientation between polycrystalline domains. For OTFT performance, blending enhances the saturation mobility from 0.22 ± 0.05 cm(2)/(V·s) (TIPS-Pentacene) to 0.72 ± 0.17 cm(2)/(V·s) (TIPS-Pentacene:PS) in addition to improving the quality of the interface between TIPS-Pentacene and the gate dielectric in the channel, resulting in threshold voltages of ∼0 V and steep subthreshold slopes.

Performance improvement of organic thin film transistors by using active layer with sandwich structure

NASA Astrophysics Data System (ADS)

Ni, Yao; Zhou, Jianlin; Kuang, Peng; Lin, Hui; Gan, Ping; Hu, Shengdong; Lin, Zhi

2017-08-01

We report organic thin film transistors (OTFTs) with pentacene/fluorinated copper phthalo-cyanine (F16CuPc)/pentacene (PFP) sandwich configuration as active layers. The sandwich devices not only show hole mobility enhancement but also present a well control about threshold voltage and off-state current. By investigating various characteristics, including current-voltage hysteresis, organic film morphology, capacitance-voltage curve and resistance variation of active layers carefully, it has been found the performance improvement is mainly attributed to the low carrier traps and the higher conductivity of the sandwich active layer due to the additional induced carriers in F16CuPc/pentacene. Therefore, using proper multiple active layer is an effective way to gain high performance OTFTs.

Charge transfer properties of pentacene adsorbed on silver: DFT study

NASA Astrophysics Data System (ADS)

N, Rekha T.; Rajkumar, Beulah J. M.

2015-06-01

Charge transfer properties of pentacene adsorbed on silver is investigated using DFT methods. Optimized geometry of pentacene after adsorption on silver indicates distortion in hexagonal structure of the ring close to the silver cluster and deviations in co-planarity of carbon atoms due to the variations in bond angles and dihedral angles. Theoretically simulated absorption spectrum has a symmetric surface plasmon resonance peak around 486nm corresponding to the transfer of charge from HOMO-2 to LUMO. Theoretical SERS confirms the process of adsorption, tilted orientation of pentacene on silver surface and the charge transfers reported. Localization of electron density arising from redistribution of electrostatic potential together with a reduced bandgap of pentacene after adsorption on silver suggests its utility in the design of electro active organic semiconducting devices.

Effect of oxygen plasma treatment on crystal growth mode at pentacene/Ni interface in organic thin-film transistors.

PubMed

Song, Bang Joo; Hong, Kihyon; Kim, Woong-Kwon; Kim, Kisoo; Kim, Sungjun; Lee, Jong-Lam

2010-11-25

We report how treatment of nickel (Ni) with O(2) plasma affects the polarity of Ni surface, crystallinity of pentacene film on the Ni, and electrical properties of pentacene organic thin-film transistors (OTFTs) that use Ni as source-drain electrodes. The polar component of surface energy in Ni surface increased from 8.1 to 43.3 mJ/m(2) after O(2)-plasma treatment for 10 s. From X-ray photoelectron spectra and secondary electron emission spectra, we found that NiO(x) was formed on the O(2)-plasma-treated Ni surface and the work function of O(2)-plasma-treated Ni was 0.85 eV higher than that of untreated Ni. X-ray diffraction and atomic force microscopy measurements showed that pentacene molecules are well aligned as a thin-film and grains grow much larger on O(2)-plasma-treated Ni than on untreated Ni. This change in the growth mode is attributed to the reduction of interaction energy between pentacene and Ni due to formation of oxide at the Ni/pentacene interface. Thus, O(2)-plasma treatment promoted the growth of well-ordered pentacene film and lowered both the hole injection barrier and the contact resistance between Ni and pentacene by forming NiO(x), enhancing the electrical property of bottom-contact OTFTs.

DNA hybridization sensor based on pentacene thin film transistor.

PubMed

Kim, Jung-Min; Jha, Sandeep Kumar; Chand, Rohit; Lee, Dong-Hoon; Kim, Yong-Sang

2011-01-15

A DNA hybridization sensor using pentacene thin film transistors (TFTs) is an excellent candidate for disposable sensor applications due to their low-cost fabrication process and fast detection. We fabricated pentacene TFTs on glass substrate for the sensing of DNA hybridization. The ss-DNA (polyA/polyT) or ds-DNA (polyA/polyT hybrid) were immobilized directly on the surface of the pentacene, producing a dramatic change in the electrical properties of the devices. The electrical characteristics of devices were studied as a function of DNA immobilization, single-stranded vs. double-stranded DNA, DNA length and concentration. The TFT device was further tested for detection of λ-phage genomic DNA using probe hybridization. Based on these results, we propose that a "label-free" detection technique for DNA hybridization is possible through direct measurement of electrical properties of DNA-immobilized pentacene TFTs. Copyright © 2010 Elsevier B.V. All rights reserved.

POLYMERIZATION AND COPOLYMERIZATION OF TETRACYANOETHYLENE UNDER THE EFFECT OF POLYMERS WITH A CONJUGATED SYSTEM,

DTIC Science & Technology

reactivity monomers such as tetracyanoethylene (I), anthracene, naphthacene and pentacene . I was polymerized alone or copolymerized with anthracene...naphthacene, or pentacene . Soluble fractions of polyphenylene or polyanthryl were used as the catalyst in various concentrations so as to vary the...magnitude as high as that of anthracene, and had an activation energy of 8-11 kcal/mol. Naphthacene, pentacene , and polyphenylene also copolymerized

Magnetic field effect on pentacene-doped sexithiophene diodes

NASA Astrophysics Data System (ADS)

Pham, Song-Toan; Fayolle, Marine; Ohto, Tatsuhiko; Tada, Hirokazu

2017-11-01

We studied the effect of impurities on the magnetoresistance of sexithiophene-based diodes using impedance spectroscopy. The impurities were introduced by doping pentacene molecules into a sexithiophene film through a co-evaporation process. The pentacene molecules act as charge-scattering centers, which trigger the negative magnetoresistance of the device. This makes it possible to tune the value of magnetoresistance from positive to negative by increasing the applied voltage. The beneficial properties induced by impurities suggest a potential route to integrate additional functions into organic devices.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mohamad, Khairul Anuar; Rusnan, Fara Naila; Seria, Dzulfahmi Mohd Husin

Investigation on the physical characterization and comparison of organic thin film based on a soluble 6,13-bis(triisopropylsilylethynyl) (TIPS) pentacene is reported. Oriented thin-films of pentacene have been successfully deposited by flow-coating method, in which the chloroform solution is sandwiched between a transparent substrate and a slide glass, followed by slow-drawing of the substrate with respect to the slide glass. Molecular orientation of flow-coated TIPS-pentacene is comparable to that of the thermal-evaporated pentacene thin film by the X-ray diffraction (XRD) results. XRD results showed that the morphology of flow-coated soluble pentacene is similar to that of the thermal-evaporated pentacene thin films inmore » series of (00l) diffraction peaks where the (001) diffraction peaks are strongest in the nominally out-of-plane intensity and interplanar spacing located at approximately 2θ = 5.33° (d-spacing, d{sub 001} = 16 Å). Following that, ITO/p-TIPS-pentacene/n-ZnO/Au vertical diode was fabricated. The diode exhibited almost linear characteristics at low voltage with nonlinear characteristics at higher voltage which similar to a pn junction behavior. The results indicated that the TIPS-pentacene semiconductor active thin films can be used as a hole injection layer for fabrication of a vertical organic transistor.« less

Spectroscopic analysis of electron trapping levels in pentacene field-effect transistors

NASA Astrophysics Data System (ADS)

Park, Chang Bum

2014-08-01

Electron trapping phenomena have been investigated with respect to the energy levels of localized trap states and bias-induced device instability effects in pentacene field-effect transistors. The mechanism of the photoinduced threshold voltage shift (ΔVT) is presented by providing a ΔVT model governed by the electron trapping. The trap-and-release behaviour functionalized by photo-irradiation also shows that the trap state for electrons is associated with the energy levels in different positions in the forbidden gap of pentacene. Spectroscopic analysis identifies two kinds of electron trap states distributed above and below the energy of 2.5 eV in the band gap of the pentacene crystal. The study of photocurrent spectra shows the specific trap levels of electrons in energy space that play a substantial role in causing device instability. The shallow and deep trapping states are distributed at two centroidal energy levels of ˜1.8 and ˜2.67 eV in the pentacene band gap. Moreover, we present a systematic energy profile of electron trap states in the pentacene crystal for the first time.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Helzel, J.; Jankowski, S.; El Helou, M.

The optical transitions of pentacene films deposited on ZnO have been studied by absorption spectroscopy as a function of temperature in the range of room temperature down to 10 K. The pentacene films were prepared with thicknesses of 10 nm, 20 nm, and 100 nm on the ZnO-O(000-1) surface by molecular beam deposition. A unique temperature dependence has been observed for the two Davydov components of the excitons for different film thicknesses. At room temperature, the energetic positions of the respective absorption bands are the same for all films, whereas the positions differ more than 20 meV at 10 Kmore » caused by the very different expansion coefficients of pentacene and ZnO. Although the pentacene is just bonded via van der Waals interaction to the ZnO substrate, the very first pentacene monolayer (adlayer) is forced to keep the initial position on the ZnO surface and suffering, therefore, a substantial tensile strain. For all the subsequent pentacene monolayers, the strain is reduced step by step resulting electronically in a strong potential gradient at the interface.« less

Air-Flow Navigated Crystal Growth for TIPS Pentacene-Based Organic Thin-Film Transistors

DOE Office of Scientific and Technical Information (OSTI.GOV)

He, Zhengran; Chen, Jihua; Sun, Zhenzhong

2012-01-01

6,13-bis(triisopropylsilylethynyl)pentacene (TIPS pentacene) is a promising active channel material of organic thin-film transistors (OTFTs) due to its solubility, stability, and high mobility. However, the growth of TIPS pentacene crystals is intrinsically anisotropic and thus leads to significant variation in the performance of OTFTs. In this paper, air flow is utilized to effectively reduce the TIPS pentacene crystal anisotropy and enhance performance consistency in OTFTs, and the resulted films are examined with optical microscopy, grazing-incidence X-ray diffraction, and thin-film transistor measurements. Under air-flow navigation (AFN), TIPS pentacene drop-cast from toluene solution has been observed to form thin films with improved crystalmore » orientation and increased areal coverage on substrates, which subsequently lead to a four-fold increase of average hole mobility and one order of magnitude enhancement in performance consistency defined by the ratio of average mobility to the standard deviation of the field-effect mobilities.« less

Impact of MoO3 interlayer on the energy level alignment of pentacene-C60 heterostructure.

PubMed

Zou, Ye; Mao, Hongying; Meng, Qing; Zhu, Daoben

2016-02-28

Using in situ ultraviolet photoelectron spectroscopy, the electronic structure evolutions at the interface between pentacene and fullerene (C60), a classical organic donor-acceptor heterostructure in organic electronic devices, on indium-tin oxide (ITO) and MoO3 modified ITO substrates have been investigated. The insertion of a thin layer MoO3 has a significant impact on the interfacial energy level alignment of pentacene-C60 heterostructure. For the deposition of C60 on pentacene, the energy difference between the highest occupied molecular orbital of donor and the lowest unoccupied molecular orbital of acceptor (HOMO(D)-LUMO(A)) offset of C60/pentacene heterostructure increased from 0.86 eV to 1.54 eV after the insertion of a thin layer MoO3 on ITO. In the inverted heterostructrure where pentacene was deposited on C60, the HOMO(D)-LUMO(A) offset of pentacene/C60 heterostructure increased from 1.32 to 2.20 eV after MoO3 modification on ITO. The significant difference of HOMO(D)-LUMO(A) offset shows the feasibility to optimize organic electronic device performance through interfacial engineering approaches, such as the insertion of a thin layer high work function MoO3 films.

Molecular adsorption and multilayer growth of pentacene on Cu(100):Layer structure and energetics

NASA Astrophysics Data System (ADS)

Satta, M.; Iacobucci, S.; Larciprete, R.

2007-04-01

We used the partial charge tight binding method to perform a full structure optimization to determine equilibrium adsorption geometries, energetics, and local charge redistribution for molecular adsorption and multilayer growth of pentacene on Cu(100). We found that single molecule adsorption induces only a localized perturbation of the metal lattice which is limited to the topmost layers. At saturation coverage four stable topologies (Brick, Wave, Lines and Zigzag) were identified, all based on pentacene molecules lying flat on the metal surface and with the central phenyl ring adsorbed in top position. Only two (Brick and Wave) out of the four structures are able to sustain multilayer growth. In both cases, assembling beyond the second layer corresponds to a transition from the flat to a tilted geometry, in which the pentacenes adopt a face-plane-face arrangement leading to a herringbone structure. The energetics of the different structure are reported as a function of the molecular number density of the pentacene multilayer by calculating cohesive, stress, and electrostatic energies. The dominant tilted molecular orientation in the pentacene multilayer is in agreement with the average tilt angle of 65° between the molecular plane and the Cu surface derived by near edge x-ray absorption spectroscopy of a four monolayer pentacene film deposited on Cu(100).

Novel Organic Field Effect Transistors via Nano-Modification

DTIC Science & Technology

2005-07-01

mobility by using two kinds of nano-scale films. One is to apply the photoalignment method on a nano-scale film to control the orientation of pentacene ...scale film (polymer electrolyte) to control moving of ions in/out an active semiconducor, pentacene or conducting polymer, for improving carrier...mobility. In this project, pentacene or a series of conducting polymers, such as the derivatives of PANI and P3HT will be patterned and manufactured in

Functional Organic Monolayers

DTIC Science & Technology

2005-10-31

Weierstall, K. Downing** and R. M. Glaeser*. J. Struct. Biol. 144, p209. 2003. 292 "A new thin-film phase of pentacene ". J. Wu and J. Spence. J...electron diffraction methods, we have discovered a new phase of pentacene , a material important for attempts to develop organic semiconductors

Electric bistability induced by incorporating self-assembled monolayers/aggregated clusters of azobenzene derivatives in pentacene-based thin-film transistors.

PubMed

Tseng, Chiao-Wei; Huang, Ding-Chi; Tao, Yu-Tai

2012-10-24

Composite films of pentacene and a series of azobenzene derivatives are prepared and used as the active channel material in top-contact, bottom-gate field-effect transistors. The transistors exhibit high field-effect mobility as well as large I-V hysteresis as a function of the gate bias history. The azobenzene moieties, incorporated either in the form of self-assembled monolayer or discrete multilayer clusters at the dielectric surface, result in electric bistability of the pentacene-based transistor either by photoexcitation or gate biasing. The direction of threshold voltage shifts, size of hysteresis, response time, and retention characteristics all strongly depend on the substituent on the benzene ring. The results show that introducing a monolayer of azobenzene moieties results in formation of charge carrier traps responsible for slower switching between the bistable states and longer retention time. With clusters of azobenzene moieties as the trap sites, the switching is faster but the retention is shorter. Detailed film structure analyses and correlation with the transistor/memory properties of these devices are provided.

Spectroscopic characterization of charged defects in polycrystalline pentacene by time- and wavelength-resolved electric force microscopy.

PubMed

Luria, Justin L; Schwarz, Kathleen A; Jaquith, Michael J; Hennig, Richard G; Marohn, John A

2011-02-01

Spatial maps of topography and trapped charge are acquired for polycrystalline pentacene thin-film transistors using electric and atomic force microscopy. In regions of trapped charge, the rate of trap clearing is studied as a function of the wavelength of incident radiation.

Interface Energy Alignment of Atomic-Layer-Deposited VOx on Pentacene: an in Situ Photoelectron Spectroscopy Investigation.

PubMed

Zhao, Ran; Gao, Yuanhong; Guo, Zheng; Su, Yantao; Wang, Xinwei

2017-01-18

Ultrathin atomic-layer-deposited (ALD) vanadium oxide (VO x ) interlayer has recently been demonstrated for remarkably reducing the contact resistance in organic electronic devices (Adv. Funct. Mater. 2016, 26, 4456). Herein, we present an in situ photoelectron spectroscopy investigation (including X-ray and ultraviolet photoelectron spectroscopies) of ALD VO x grown on pentacene to understand the role of the ALD VO x interlayer for the improved contact resistance. The in situ photoelectron spectroscopy characterizations allow us to monitor the ALD growth process of VO x and trace the evolutions of the work function, pentacene HOMO level, and VO x defect states during the growth. The initial VO x growth is found to be partially delayed on pentacene in the first ∼20 ALD cycles. The underneath pentacene layer is largely intact after ALD. The ALD VO x is found to contain a high density of defect states starting from 0.67 eV below the Fermi level, and the energy level of these defect states is in excellent alignment with the HOMO level of pentacene, which therefore allows these VO x defect states to provide an efficient hole-injection pathway at the contact interface.

Epitaxial pentacene films grown on the surface of ion-beam-processed gate dielectric layer

NASA Astrophysics Data System (ADS)

Chou, W. Y.; Kuo, C. W.; Cheng, H. L.; Mai, Y. S.; Tang, F. C.; Lin, S. T.; Yeh, C. Y.; Horng, J. B.; Chia, C. T.; Liao, C. C.; Shu, D. Y.

2006-06-01

The following research describes the process of fabrication of pentacene films with submicron thickness, deposited by thermal evaporation in high vacuum. The films were fabricated with the aforementioned conditions and their characteristics were analyzed using x-ray diffraction, scanning electron microscopy, polarized Raman spectroscopy, and photoluminescence. Organic thin-film transistors (OTFTs) were fabricated on an indium tin oxide coated glass substrate, using an active layer of ordered pentacene molecules, which were grown at room temperature. Pentacene film was aligned using the ion-beam aligned method, which is typically employed to align liquid crystals. Electrical measurements taken on a thin-film transistor indicated an increase in the saturation current by a factor of 15. Pentacene-based OTFTs with argon ion-beam-processed gate dielectric layers of silicon dioxide, in which the direction of the ion beam was perpendicular to the current flow, exhibited a mobility that was up to an order of magnitude greater than that of the controlled device without ion-beam process; current on/off ratios of approximately 106 were obtained. Polarized Raman spectroscopy investigation indicated that the surface of the gate dielectric layer, treated with argon ion beam, enhanced the intermolecular coupling of pentacene molecules. The study also proposes the explanation for the mechanism of carrier transportation in pentacene films.

DOE Office of Scientific and Technical Information (OSTI.GOV)

N, Rekha T.; Rajkumar, Beulah J. M., E-mail: beulah-rajkumar@yahoo.co.in

Charge transfer properties of pentacene adsorbed on silver is investigated using DFT methods. Optimized geometry of pentacene after adsorption on silver indicates distortion in hexagonal structure of the ring close to the silver cluster and deviations in co-planarity of carbon atoms due to the variations in bond angles and dihedral angles. Theoretically simulated absorption spectrum has a symmetric surface plasmon resonance peak around 486nm corresponding to the transfer of charge from HOMO-2 to LUMO. Theoretical SERS confirms the process of adsorption, tilted orientation of pentacene on silver surface and the charge transfers reported. Localization of electron density arising from redistributionmore » of electrostatic potential together with a reduced bandgap of pentacene after adsorption on silver suggests its utility in the design of electro active organic semiconducting devices.« less

Effect of Pentacene-dielectric Affinity on Pentacene Thin Film Growth Morphology in Organic Field-effect Transistors

DOE Office of Scientific and Technical Information (OSTI.GOV)

S Kim; M Jang; H Yang

2011-12-31

Organic field-effect transistors (OFETs) are fabricated by depositing a thin film of semiconductor on the functionalized surface of a SiO{sub 2} dielectric. The chemical and morphological structures of the interface between the semiconductor and the functionalized dielectric are critical for OFET performance. We have characterized the effect of the affinity between semiconductor and functionalized dielectric on the properties of the semiconductor-dielectric interface. The crystalline microstructure/nanostructure of the pentacene semiconductor layers, grown on a dielectric substrate that had been functionalized with either poly(4-vinyl pyridine) or polystyrene (to control hydrophobicity), and grown under a series of substrate temperatures and deposition rates, weremore » characterized by X-ray diffraction, photoemission spectroscopy, and atomic force microscopy. By comparing the morphological features of the semiconductor thin films with the device characteristics (field-effect mobility, threshold voltage, and hysteresis) of the OFET devices, the effect of affinity-driven properties on charge modulation, charge trapping, and charge carrier transport could be described.« less

Contact-metal dependent current injection in pentacene thin-film transistors

NASA Astrophysics Data System (ADS)

Wang, S. D.; Minari, T.; Miyadera, T.; Tsukagoshi, K.; Aoyagi, Y.

2007-11-01

Contact-metal dependent current injection in top-contact pentacene thin-film transistors is analyzed, and the local mobility in the contact region was found to follow the Meyer-Neldel rule. An exponential trap distribution, rather than the metal/organic hole injection barrier, is proposed to be the dominant factor of the contact resistance in pentacene thin-film transistors. The variable temperature measurements revealed a much narrower trap distribution in the copper contact compared with the corresponding gold contact, and this is the origin of the smaller contact resistance for copper despite a lower work function.

Wannier-function-based constrained DFT with nonorthogonality-correcting Pulay forces in application to the reorganization effects in graphene-adsorbed pentacene

NASA Astrophysics Data System (ADS)

Roychoudhury, Subhayan; O'Regan, David D.; Sanvito, Stefano

2018-05-01

Pulay terms arise in the Hellmann-Feynman forces in electronic-structure calculations when one employs a basis set made of localized orbitals that move with their host atoms. If the total energy of the system depends on a subspace population defined in terms of the localized orbitals across multiple atoms, then unconventional Pulay terms will emerge due to the variation of the orbital nonorthogonality with ionic translation. Here, we derive the required exact expressions for such terms, which cannot be eliminated by orbital orthonormalization. We have implemented these corrected ionic forces within the linear-scaling density functional theory (DFT) package onetep, and we have used constrained DFT to calculate the reorganization energy of a pentacene molecule adsorbed on a graphene flake. The calculations are performed by including ensemble DFT, corrections for periodic boundary conditions, and empirical Van der Waals interactions. For this system we find that tensorially invariant population analysis yields an adsorbate subspace population that is very close to integer-valued when based upon nonorthogonal Wannier functions, and also but less precisely so when using pseudoatomic functions. Thus, orbitals can provide a very effective population analysis for constrained DFT. Our calculations show that the reorganization energy of the adsorbed pentacene is typically lower than that of pentacene in the gas phase. We attribute this effect to steric hindrance.

Trap densities and transport properties of pentacene metal-oxide-semiconductor transistors. I. Analytical modeling of time-dependent characteristics

NASA Astrophysics Data System (ADS)

Basile, A. F.; Cramer, T.; Kyndiah, A.; Biscarini, F.; Fraboni, B.

2014-06-01

Metal-oxide-semiconductor (MOS) transistors fabricated with pentacene thin films were characterized by temperature-dependent current-voltage (I-V) characteristics, time-dependent current measurements, and admittance spectroscopy. The channel mobility shows almost linear variation with temperature, suggesting that only shallow traps are present in the semiconductor and at the oxide/semiconductor interface. The admittance spectra feature a broad peak, which can be modeled as the sum of a continuous distribution of relaxation times. The activation energy of this peak is comparable to the polaron binding energy in pentacene. The absence of trap signals in the admittance spectra confirmed that both the semiconductor and the oxide/semiconductor interface have negligible density of deep traps, likely owing to the passivation of SiO2 before pentacene growth. Nevertheless, current instabilities were observed in time-dependent current measurements following the application of gate-voltage pulses. The corresponding activation energy matches the energy of a hole trap in SiO2. We show that hole trapping in the oxide can explain both the temperature and the time dependences of the current instabilities observed in pentacene MOS transistors. The combination of these experimental techniques allows us to derive a comprehensive model for charge transport in hybrid architectures where trapping processes occur at various time and length scales.

High-Mobility 6,13-Bis(triisopropylsilylethynyl) Pentacene Transistors Using Solution-Processed Polysilsesquioxane Gate Dielectric Layers.

PubMed

Matsuda, Yu; Nakahara, Yoshio; Michiura, Daisuke; Uno, Kazuyuki; Tanaka, Ichiro

2016-04-01

Polysilsesquioxane (PSQ) is a low-temperature curable polymer that is compatible with low-cost plastic substrates. We cured PSQ gate dielectric layers by irradiation with ultraviolet light at ~60 °C, and used them for 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS-pentacene) thin film transistors (TFTs). The fabricated TFTs have shown the maximum and average hole mobility of 1.3 and 0.78 ± 0.3 cm2V-1s-1, which are comparable to those of the previously reported transistors using single-crystalline TIPS-pentacene micro-ribbons for their active layers and thermally oxidized SiO2 for their gate dielectric layers. Itis therefore demonstrated that PSQ is a promising polymer gate dielectric material for low-cost organic TFTs.

Preparation of pentacene thin film deposited using organic material auto-feeding system for the fabrication of organic thin film transistor.

PubMed

Kim, Young Baek; Choi, Bum Ho; Lim, Yong Hwan; Yoo, Ha Na; Lee, Jong Ho; Kim, Jin Hyeok

2011-02-01

In this study, pentacene organic thin film was prepared using newly developed organic material auto-feeding system integrated with linear cell and characterized. The newly developed organic material auto-feeding system consists of 4 major parts: reservoir, micro auto-feeder, vaporizer, and linear cell. The deposition of organic thin film could be precisely controlled by adjusting feeding rate, main tube size, position and size of nozzle. 10 nm thick pentacene thin film prepared on glass substrate exhibited high uniformity of 3.46% which is higher than that of conventional evaporation method using point cell. The continuous deposition without replenishment of organic material can be performed over 144 hours with regulated deposition control. The grain size of pentacene film which affect to mobility of OTFT, was controlled as a function of the temperature.

Charge transport calculations by a wave-packet dynamical approach using maximally localized Wannier functions based on density functional theory: Application to high-mobility organic semiconductors

NASA Astrophysics Data System (ADS)

Ishii, Hiroyuki; Kobayashi, Nobuhiko; Hirose, Kenji

2017-01-01

We present a wave-packet dynamical approach to charge transport using maximally localized Wannier functions based on density functional theory including van der Waals interactions. We apply it to the transport properties of pentacene and rubrene single crystals and show the temperature-dependent natures from bandlike to thermally activated behaviors as a function of the magnitude of external static disorder. We compare the results with those obtained by the conventional band and hopping models and experiments.

FAR-INFRARED SPECTROSCOPY OF CATIONIC POLYCYCLIC AROMATIC HYDROCARBONS: ZERO KINETIC ENERGY PHOTOELECTRON SPECTROSCOPY OF PENTACENE VAPORIZED FROM LASER DESORPTION

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang Jie; Han Fangyuan; Pei Linsen

2010-05-20

The distinctive set of infrared (IR) emission bands at 3.3, 6.2, 7.7, 8.6, and 11.3 {mu}m are ubiquitously seen in a wide variety of astrophysical environments. They are generally attributed to polycyclic aromatic hydrocarbon (PAH) molecules. However, not a single PAH species has yet been identified in space, as the mid-IR vibrational bands are mostly representative of functional groups and thus do not allow one to fingerprint individual PAH molecules. In contrast, the far-IR (FIR) bands are sensitive to the skeletal characteristics of a molecule, hence they are important for chemical identification of unknown species. With an aim to offermore » laboratory astrophysical data for the Herschel Space Observatory, Stratospheric Observatory for Infrared Astronomy, and similar future space missions, in this work we report neutral and cation FIR spectroscopy of pentacene (C{sub 22}H{sub 14}), a five-ring PAH molecule. We report three IR active modes of cationic pentacene at 53.3, 84.8, and 266 {mu}m that may be detectable by space missions such as the SAFARI instrument on board SPICA. In the experiment, pentacene is vaporized from a laser desorption source and cooled by a supersonic argon beam. We have obtained results from two-color resonantly enhanced multiphoton ionization and two-color zero kinetic energy photoelectron (ZEKE) spectroscopy. Several skeletal vibrational modes of the first electronically excited state of the neutral species and those of the cation are assigned, with the aid of ab initio and density functional calculations. Although ZEKE is governed by the Franck-Condon principle different from direct IR absorption or emission, vibronic coupling in the long ribbon-like molecule results in the observation of a few IR active modes. Within the experimental resolution of {approx}7 cm{sup -1}, the frequency values from our calculation agree with the experiment for the cation, but differ for the electronically excited intermediate state. Consequently, modeling of the intensity distribution is difficult and may require explicit inclusion of vibronic interactions.« less

The anchoring effect on the spin transport properties and I-V characteristics of pentacene molecular devices suspended between nickel electrodes.

PubMed

Caliskan, S; Laref, A

2014-07-14

Spin-polarized transport properties are determined for pentacene sandwiched between Ni surface electrodes with various anchoring ligands. These calculations are carried out using spin density functional theory in tandem with a non-equilibrium Green's function technique. The presence of a Se atom at the edge of the pentacene molecule significantly modifies the transport properties of the device because Se has a different electronegativity than S. Our theoretical results clearly show a larger current for spin-up electrons than for spin-down electrons in the molecular junction that is attached asymmetrically across the Se linker at one side of the Ni electrodes (in an APL magnetic orientation). Moreover, this molecular junction exhibits pronounced NDR as the bias voltage is increased from 0.8 to 1.0 V. However, this novel NDR behavior is only detected in this promising pentacene molecular device. The NDR in the current-voltage (I-V) curve results from the narrowness of the density of states for the molecular states. The feasibility of controlling the TMR is also predicted in these molecular device nanostructures. Spin-dependent transmission calculations show that the sign and strength of the current-bias voltage characteristics and the TMR could be tailored for the organic molecule devices. These molecular junctions are joined symmetrically and asymmetrically between Ni metallic probes across the S and Se atoms (at the ends of the edges of the pentacene molecule). Our theoretical findings show that spin-valve phenomena can occur in these prototypical molecular junctions. The TMR and NDR results show that nanoscale junctions with spin valves could play a vital role in the production of novel functional molecular devices.

An In Silico Study on the Isomers of Pentacene: The Case for Air-Stable and Alternative C22H14 Acenes for Organic Electronics.

PubMed

Jones, Leighton; Lin, Long

2017-04-13

Pentacene is one of the most investigated candidates for organic thin film transistor (OTFT) applications over the last few decades even though it unstable in air (E g = 1.80 eV), owing in part to its planar nature and high charge-transfer mobilities as both a single crystal (35 cm 2 V -1 s -1 ) and as a thin-film (3.0 cm 2 V -1 s -1 ). Until now, picene is the only isomer of pentacene to be investigated for organic electronic applications, due to its greater stability (E g = 4.21 eV) and high-charge transfer mobility (3.0 cm 2 V -1 s -1 ); even benefiting from oxygen doping. In the present study, a total of 12 fused-ring isomers (including pentacene, picene and ten other structures) of the formula C 22 H 14 were analyzed and investigated for their electronic and optical properties for worth in OTFT applications. We screened several pure and hybrid DFT functionals against the experimental frontier molecular orbitals (FMOs) of pentacene, then deployed Marcus Theory, Koopmans' Theorem and Green's function with the P3 electron propagator variant, for the internal hole reorganization energy, the hole transfer integral (via the "splitting-in-dimer method" at d = 3.0, 3.5, and 4.0 Å), the charge transfer rate constant, and vertical ionization energies. Using these as a basis, we studied pentacene's isomers and found that the four nonplanar structures, namely, benzo[g]chrysene (3), naphtho[c]phenanthrene (7), benzo[c]chrysene (11) and dibenzo[c,c']phenthrene (12), are (I) more stable than pentacene, by up to 2 eV, and (II) have relatively similar ionization energies (7.5-7.6 eV) to those of picene's experimental value (7.51 eV). The largest charge transfer rates at 3.5 Å dimer separations were given by the isomers benzo[b]chrysene 4, naphtha[c]phenanthrene 7, dibenzo[a,c]anthracene 8 and benzo[a]tetracene 10 and found to be 2.92, 1.72, 1.30, and 3.09 × 10 14 s -1 respectively. In comparison to that of pentacene (K CT = 3.97 × 10 14 s -1 ), these unusual isomers are thus promising air-stable and alternative candidates for organic electronic applications.

Combined UMC- DFT prediction of electron-hole coupling in unit cells of pentacene crystals.

PubMed

Leal, Luciano Almeida; de Souza Júnior, Rafael Timóteo; de Almeida Fonseca, Antonio Luciano; Ribeiro Junior, Luiz Antonio; Blawid, Stefan; da Silva Filho, Demetrio Antonio; da Cunha, Wiliam Ferreira

2017-05-01

Pentacene is an organic semiconductor that draws special attention from the scientific community due to the high mobility of its charge carriers. As electron-hole interactions are important aspects in the regard of such property, a computationally inexpensive method to predict the coupling between these quasi-particles is highly desired. In this work, we propose a hybrid methodology of combining Uncoupled Monte Carlo Simulations (UMC) and Density functional Theory (DFT) methodologies to obtain a good compromise between computational feasibility and accuracy. As a first step in considering a Pentacene crystal, we describe its unit cell: the Pentacene Dimer. Because many conformations can be encountered for the dimer and considering the complexity of the system, we make use of UMC in order to find the most probable structures and relative orientations for the Pentacene-Pentacene complex. Following, we carry out electronic structure calculations in the scope of DFT with the goal of describing the electron-hole coupling on the most probable configurations obtained by UMC. The comparison of our results with previously reported data on the literature suggests that the methodology is well suited for describing transfer integrals of organic semiconductors. The observed accuracy together with the smaller computational cost required by our approach allows us to conclude that such methodology might be an important tool towards the description of systems with higher complexity.

Explicit crystal host effects on excited state properties of linear polyacenes: towards a room-temperature maser

NASA Astrophysics Data System (ADS)

Charlton, Robert; Bogatko, Stuart; Zuehlsdorff, Tim; Hine, Nicholas; Horsfield, Andrew; Haynes, Peter

Maser technology has been held back for decades by the impracticality of the operating conditions of traditional masing devices, such as cryogenic freezing and strong magnetic fields. Recently it has been experimentally demonstrated that pentacene in p-terphenyl can act as a viable solid-state room-temperature maser by exploiting the alignment of the low-lying singlet and triplet excited states of pentacene. To understand the operation of this device from first principles, an ab initio study of the excitonic properties of pentacene in p-terphenyl has been carried out using time-dependent density functional theory (TDDFT), implemented in the linear-scaling ONETEP software (www.onetep.org). In particular, we focus on the impact that the wider crystal has on the localised pentacene excitations by performing an explicit DFT treatment of the p-terphenyl environment. We demonstrate the importance of explicit crystal host effects in calculating the excitation energies of pentacene in p-terphenyl, providing important information for the operation of the maser. We then use this same approach to test the viability of other linear polyacenes as maser candidates as a screening step before experimental testing.

How lithium atoms affect the first hyperpolarizability of BN edge-doped graphene.

PubMed

Song, Yao-Dong; Wu, Li-Ming; Chen, Qiao-Ling; Liu, Fa-Kun; Tang, Xiao-Wen

2016-01-01

How do lithium atoms affect the first hyperpolarizability (β0) of boron-nitrogen (BN) edge-doped graphene. In this work, using pentacene as graphene model, Lin@BN-1 edge-doped pentacene and Lin@BN-2 edge-doped pentacene (n = 1, 5) were designed to study this problem. First, two models (BN-1 edge-doped pentacene, and BN-2 edge-doped pentacene ) were formed by doping the BN into the pentacene with different order, and then Li@BN-1 edge-doped pentacene and Li@ BN-2 edge-doped pentacene were obtained by substituting the H atom in BN edge-doped pentacene with a Li atom. The results show that the first hyperpolarizabilities of BN-1 edge-doped pentacene and Li@BN-1 edge-doped pentacene were 4059 a.u. and 6249 a.u., respectively; the first hyperpolarizabilities of BN-2 edge-doped pentacene and Li@BN-2 edge-doped pentacene were 2491 a.u. and 4265 a.u., respectively. The results indicate that the effect of Li substitution is to greatly increase the β0 value. To further enhance the first hyperpolarizability, Li5@ BN-1 edge-doped pentacene and Li5@BN-2 edge-doped pentacene were designed, and were found to exhibit considerably larger first hyperpolarizabilities (β0) (12,112 a.u. and 7921a.u., respectively). This work may inspire further study of the nonlinear properties of BN edge-doped graphene.

Subthreshold characteristics of pentacene field-effect transistors influenced by grain boundaries

NASA Astrophysics Data System (ADS)

Park, Jaehoon; Jeong, Ye-Sul; Park, Kun-Sik; Do, Lee-Mi; Bae, Jin-Hyuk; Sun Choi, Jong; Pearson, Christopher; Petty, Michael

2012-05-01

Grain boundaries in polycrystalline pentacene films significantly affect the electrical characteristics of pentacene field-effect transistors (FETs). Upon reversal of the gate voltage sweep direction, pentacene FETs exhibited hysteretic behaviours in the subthreshold region, which was more pronounced for the FET having smaller pentacene grains. No shift in the flat-band voltage of the metal-insulator-semiconductor capacitor elucidates that the observed hysteresis was mainly caused by the influence of localized trap states existing at pentacene grain boundaries. From the results of continuous on/off switching operation of the pentacene FETs, hole depletion during the off period is found to be limited by pentacene grain boundaries. It is suggested that the polycrystalline nature of a pentacene film plays an important role on the dynamic characteristics of pentacene FETs.

Picosecond Transient Photoconductivity in Functionalized Pentacene Molecular Crystals Probed by Terahertz Pulse Spectroscopy

NASA Astrophysics Data System (ADS)

Hegmann, F. A.; Tykwinski, R. R.; Lui, K. P.; Bullock, J. E.; Anthony, J. E.

2002-11-01

We have measured transient photoconductivity in functionalized pentacene molecular crystals using ultrafast optical pump-terahertz probe techniques. The single crystal samples were excited using 800nm, 100fs pulses, and the change in transmission of time-delayed, subpicosecond terahertz pulses was used to probe the photoconducting state over a temperature range from 10 to 300K. A subpicosecond rise in photoconductivity is observed, suggesting that mobile carriers are a primary photoexcitation. At times longer than 4ps, a power-law decay is observed consistent with dispersive transport.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yun, Dong-Jin; Chung, JaeGwan; Jung, Changhoon

The material arrangement and energy level alignment of an organic bilayer comprising of phenyl-c71-butyric-acid-methyl ester (PCBM-71) and pentacene were studied using ultraviolet photoelectron spectroscopy (UPS) and the argon gas cluster ion beam (GCIB) sputtering process. Although there is a small difference in the full width at half maximum of the carbon C 1s core level peaks and differences in the oxygen O 1s core levels of an X-ray photoemission spectroscopy spectra, these differences are insufficient to clearly distinguish between PCBM-71 and pentacene layers and to classify the interface and bulk regions. On the other hand, the valence band structures inmore » the UPS spectra contain completely distinct configurations for the PCBM-71 and pentacene layers, even when they have similar atomic compositions. According to the valence band structures of the PCBM-71/pentacene/electrodes, the highest unoccupied molecular orbital (HOMO) region of pentacene is at least 0.8 eV closer to the Fermi level than that of PCBM-71 and it does not overlap with any of the chemical states in the valence band structure of PCBM-71. Therefore, by just following the variations in the area of the HOMO region of pentacene, the interface/bulk regions of the PCBM/pentacene layers were distinctly categorized. Besides, the variation of valence band structures as a function of the Ar GCIB sputtering time fully corroborated with the surface morphologies observed in the atomic force microscope images. In summary, we believe that the novel approach, which involves UPS analysis in conjunction with Ar GCIB sputtering, can be one of the best methods to characterize the material distribution and energy level alignments of stacks of organic layers.« less

Formation and electrical transport properties of pentacene nanorod crystal.

PubMed

Akai-Kasaya, M; Ohmori, C; Kawanishi, T; Nashiki, M; Saito, A; Aono, M; Kuwahara, Y

2010-09-10

The monophasic formation of an uncharted pentacene crystal, the pentacene nanorod, has been investigated. The restricted formation of the pentacene nanorod on a bare mica surface reveals a peculiar surface catalytic crystal growth mode of the pentacene. We demonstrated the charge transport measurements through a single pentacene nanorod and analyzed the data using a periodic hopping conduction model. The results revealed that the pentacene nanorod has a periodic conductive node within their one-dimensional crystal.

Quantitative evaluation of spatial scale of carrier trapping at grain boundary by GHz-microwave dielectric loss spectroscopy

NASA Astrophysics Data System (ADS)

Choi, W.; Tsutsui, Y.; Miyakai, T.; Sakurai, T.; Seki, S.

2017-11-01

Charge carrier mobility is an important primary parameter for the electronic conductive materials, and the intrinsic limit of the mobility has been hardly access by conventional direct-current evaluation methods. In the present study, intra-grain hole mobility of pentacene thin films was estimated quantitatively using microwave-based dielectric loss spectroscopy (time-resolved microwave conductivity measurement) in alternating current mode of charge carrier local motion. Metal-insulator-semiconductor devices were prepared with different insulating polymers or substrate temperature upon vacuum deposition of the pentacene layer, which afforded totally four different grain-size conditions of pentacene layers. Under the condition where the local motion was determined by interfacial traps at the pentacene grain boundaries (grain-grain interfaces), the observed hole mobilities were plotted against the grain sizes, giving an excellent correlation fit successfully by a parabolic function representative of the boarder length. Consequently, the intra-grain mobility and trap-release time of holes were estimated as 15 cm2 V-1 s-1 and 9.4 ps.

In situ preparation, electrical and surface analytical characterization of pentacene thin film transistors

PubMed Central

Lassnig, R.; Striedinger, B.; Hollerer, M.; Fian, A.; Stadlober, B.; Winkler, A.

2015-01-01

The fabrication of organic thin film transistors with highly reproducible characteristics presents a very challenging task. We have prepared and analyzed model pentacene thin film transistors under ultra-high vacuum conditions, employing surface analytical tools and methods. Intentionally contaminating the gold contacts and SiO2 channel area with carbon through repeated adsorption, dissociation, and desorption of pentacene proved to be very advantageous in the creation of devices with stable and reproducible parameters. We mainly focused on the device properties, such as mobility and threshold voltage, as a function of film morphology and preparation temperature. At 300 K, pentacene displays Stranski-Krastanov growth, whereas at 200 K fine-grained, layer-like film growth takes place, which predominantly influences the threshold voltage. Temperature dependent mobility measurements demonstrate good agreement with the established multiple trapping and release model, which in turn indicates a predominant concentration of shallow traps in the crystal grains and at the oxide-semiconductor interface. Mobility and threshold voltage measurements as a function of coverage reveal that up to four full monolayers contribute to the overall charge transport. A significant influence on the effective mobility also stems from the access resistance at the gold contact-semiconductor interface, which is again strongly influenced by the temperature dependent, characteristic film growth mode. PMID:25814770

In situ preparation, electrical and surface analytical characterization of pentacene thin film transistors

NASA Astrophysics Data System (ADS)

Lassnig, R.; Striedinger, B.; Hollerer, M.; Fian, A.; Stadlober, B.; Winkler, A.

2014-09-01

The fabrication of organic thin film transistors with highly reproducible characteristics presents a very challenging task. We have prepared and analyzed model pentacene thin film transistors under ultra-high vacuum conditions, employing surface analytical tools and methods. Intentionally contaminating the gold contacts and SiO2 channel area with carbon through repeated adsorption, dissociation, and desorption of pentacene proved to be very advantageous in the creation of devices with stable and reproducible parameters. We mainly focused on the device properties, such as mobility and threshold voltage, as a function of film morphology and preparation temperature. At 300 K, pentacene displays Stranski-Krastanov growth, whereas at 200 K fine-grained, layer-like film growth takes place, which predominantly influences the threshold voltage. Temperature dependent mobility measurements demonstrate good agreement with the established multiple trapping and release model, which in turn indicates a predominant concentration of shallow traps in the crystal grains and at the oxide-semiconductor interface. Mobility and threshold voltage measurements as a function of coverage reveal that up to four full monolayers contribute to the overall charge transport. A significant influence on the effective mobility also stems from the access resistance at the gold contact-semiconductor interface, which is again strongly influenced by the temperature dependent, characteristic film growth mode.

Effects of the F₄TCNQ-Doped Pentacene Interlayers on Performance Improvement of Top-Contact Pentacene-Based Organic Thin-Film Transistors.

PubMed

Fan, Ching-Lin; Lin, Wei-Chun; Chang, Hsiang-Sheng; Lin, Yu-Zuo; Huang, Bohr-Ran

2016-01-13

In this paper, the top-contact (TC) pentacene-based organic thin-film transistor (OTFT) with a tetrafluorotetracyanoquinodimethane (F₄TCNQ)-doped pentacene interlayer between the source/drain electrodes and the pentacene channel layer were fabricated using the co-evaporation method. Compared with a pentacene-based OTFT without an interlayer, OTFTs with an F₄TCNQ:pentacene ratio of 1:1 showed considerably improved electrical characteristics. In addition, the dependence of the OTFT performance on the thickness of the F₄TCNQ-doped pentacene interlayer is weaker than that on a Teflon interlayer. Therefore, a molecular doping-type F₄TCNQ-doped pentacene interlayer is a suitable carrier injection layer that can improve the TC-OTFT performance and facilitate obtaining a stable process window.

Different interface orientations of pentacene and PTCDA induce different degrees of disorder

PubMed Central

2012-01-01

Organic polymers or crystals are commonly used in manufacturing of today‘s electronically functional devices (OLEDs, organic solar cells, etc). Understanding their morphology in general and at the interface in particular is of paramount importance. Proper knowledge of molecular orientation at interfaces is essential for predicting optoelectronic properties such as exciton diffusion length, charge carrier mobility, and molecular quadrupole moments. Two promising candidates are pentacene and 3,4:9,10-perylenetetracarboxylic dianhydride (PTCDA). Different orientations of pentacene on PTCDA have been investigated using an atomistic molecular dynamics approach. Here, we show that the degree of disorder at the interface depends largely on the crystal orientation and that more ordered interfaces generally suffer from large vacancy formation. PMID:22583772

Implicit and explicit host effects on excitons in pentacene derivatives.

PubMed

Charlton, R J; Fogarty, R M; Bogatko, S; Zuehlsdorff, T J; Hine, N D M; Heeney, M; Horsfield, A P; Haynes, P D

2018-03-14

An ab initio study of the effects of implicit and explicit hosts on the excited state properties of pentacene and its nitrogen-based derivatives has been performed using ground state density functional theory (DFT), time-dependent DFT, and ΔSCF. We observe a significant solvatochromic redshift in the excitation energy of the lowest singlet state (S 1 ) of pentacene from inclusion in a p-terphenyl host compared to vacuum; for an explicit host consisting of six nearest neighbour p-terphenyls, we obtain a redshift of 65 meV while a conductor-like polarisable continuum model (CPCM) yields a 78 meV redshift. Comparison is made between the excitonic properties of pentacene and four of its nitrogen-based analogs, 1,8-, 2,9-, 5,12-, and 6,13-diazapentacene with the latter found to be the most distinct due to local distortions in the ground state electronic structure. We observe that a CPCM is insufficient to fully understand the impact of the host due to the presence of a mild charge-transfer (CT) coupling between the chromophore and neighbouring p-terphenyls, a phenomenon which can only be captured using an explicit model. The strength of this CT interaction increases as the nitrogens are brought closer to the central acene ring of pentacene.

Implicit and explicit host effects on excitons in pentacene derivatives

NASA Astrophysics Data System (ADS)

Charlton, R. J.; Fogarty, R. M.; Bogatko, S.; Zuehlsdorff, T. J.; Hine, N. D. M.; Heeney, M.; Horsfield, A. P.; Haynes, P. D.

2018-03-01

An ab initio study of the effects of implicit and explicit hosts on the excited state properties of pentacene and its nitrogen-based derivatives has been performed using ground state density functional theory (DFT), time-dependent DFT, and ΔSCF. We observe a significant solvatochromic redshift in the excitation energy of the lowest singlet state (S1) of pentacene from inclusion in a p-terphenyl host compared to vacuum; for an explicit host consisting of six nearest neighbour p-terphenyls, we obtain a redshift of 65 meV while a conductor-like polarisable continuum model (CPCM) yields a 78 meV redshift. Comparison is made between the excitonic properties of pentacene and four of its nitrogen-based analogs, 1,8-, 2,9-, 5,12-, and 6,13-diazapentacene with the latter found to be the most distinct due to local distortions in the ground state electronic structure. We observe that a CPCM is insufficient to fully understand the impact of the host due to the presence of a mild charge-transfer (CT) coupling between the chromophore and neighbouring p-terphenyls, a phenomenon which can only be captured using an explicit model. The strength of this CT interaction increases as the nitrogens are brought closer to the central acene ring of pentacene.

Effects of the F4TCNQ-Doped Pentacene Interlayers on Performance Improvement of Top-Contact Pentacene-Based Organic Thin-Film Transistors

PubMed Central

Fan, Ching-Lin; Lin, Wei-Chun; Chang, Hsiang-Sheng; Lin, Yu-Zuo; Huang, Bohr-Ran

2016-01-01

In this paper, the top-contact (TC) pentacene-based organic thin-film transistor (OTFT) with a tetrafluorotetracyanoquinodimethane (F4TCNQ)-doped pentacene interlayer between the source/drain electrodes and the pentacene channel layer were fabricated using the co-evaporation method. Compared with a pentacene-based OTFT without an interlayer, OTFTs with an F4TCNQ:pentacene ratio of 1:1 showed considerably improved electrical characteristics. In addition, the dependence of the OTFT performance on the thickness of the F4TCNQ-doped pentacene interlayer is weaker than that on a Teflon interlayer. Therefore, a molecular doping-type F4TCNQ-doped pentacene interlayer is a suitable carrier injection layer that can improve the TC-OTFT performance and facilitate obtaining a stable process window. PMID:28787845

Origins of Singlet Fission in Solid Pentacene from an ab initio Green's Function Approach

NASA Astrophysics Data System (ADS)

Refaely-Abramson, Sivan; da Jornada, Felipe H.; Louie, Steven G.; Neaton, Jeffrey B.

2017-12-01

We develop a new first-principles approach to predict and understand rates of singlet fission with an ab initio Green's-function formalism based on many-body perturbation theory. Starting with singlet and triplet excitons computed from a G W plus Bethe-Salpeter equation approach, we calculate the exciton-biexciton coupling to lowest order in the Coulomb interaction, assuming a final state consisting of two noninteracting spin-correlated triplets with finite center-of-mass momentum. For crystalline pentacene, symmetries dictate that the only purely Coulombic fission decay process from a bright singlet state requires a final state consisting of two inequivalent nearly degenerate triplets of nonzero, equal and opposite, center-of-mass momenta. For such a process, we predict a singlet lifetime of 30-70 fs, in very good agreement with experimental data, indicating that this process can dominate singlet fission in crystalline pentacene. Our approach is general and provides a framework for predicting and understanding multiexciton interactions in solids.

Adsorption and electronic properties of pentacene on thin dielectric decoupling layers.

PubMed

Koslowski, Sebastian; Rosenblatt, Daniel; Kabakchiev, Alexander; Kuhnke, Klaus; Kern, Klaus; Schlickum, Uta

2017-01-01

With the increasing use of thin dielectric decoupling layers to study the electronic properties of organic molecules on metal surfaces, comparative studies are needed in order to generalize findings and formulate practical rules. In this paper we study the adsorption and electronic properties of pentacene deposited onto h-BN/Rh(111) and compare them with those of pentacene deposited onto KCl on various metal surfaces. When deposited onto KCl, the HOMO and LUMO energies of the pentacene molecules scale with the work functions of the combined KCl/metal surface. The magnitude of the variation between the respective KCl/metal systems indicates the degree of interaction of the frontier orbitals with the underlying metal. The results confirm that the so-called IDIS model developed by Willenbockel et al. applies not only to molecular layers on bare metal surfaces, but also to individual molecules on thin electronically decoupling layers. Depositing pentacene onto h-BN/Rh(111) results in significantly different adsorption characteristics, due to the topographic corrugation of the surface as well as the lateral electric fields it presents. These properties are reflected in the divergence from the aforementioned trend for the orbital energies of pentacene deposited onto h-BN/Rh(111), as well as in the different adsorption geometry. Thus, the highly desirable capacity of h-BN to trap molecules comes at the price of enhanced metal-molecule interaction, which decreases the HOMO-LUMO gap of the molecules. In spite of the enhanced interaction, the molecular orbitals are evident in scanning tunnelling spectroscopy (STS) and their shapes can be resolved by spectroscopic mapping.

Evidence for spin injection and transport in solution-processed TIPS-pentacene at room temperature

NASA Astrophysics Data System (ADS)

Mooser, S.; Cooper, J. F. K.; Banger, K. K.; Wunderlich, J.; Sirringhaus, H.

2012-10-01

Recently, there has been growing interest in the field of organic spintronics, where the research on organic semiconductors (OSCs) has extended from the complex aspects of charge carrier transport to the study of the spin transport properties of those anisotropic and partly localized systems.1 Furthermore, solution-processed OSCs are not only interesting due to their technological applications, but it has recently been shown in 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS-pentacene) thin film transistors that they can exhibit a negative temperature coefficient of the mobility due to localized transport limited by thermal lattice fluctuations.2 Here, spin injection and transport in solution-processed TIPS-pentacene are investigated exploiting vertical CoPt/TIPSpentacene/AlOx/Co spin valve architectures.3 The antiparallel magnetization state of the relative orientation of CoPt and Co is achieved due to their different coercive fields. A spin valve effect is detected from T = 175 K up to room temperature, where the resistance of the device is lower for the antiparallel magnetization state. The first observation of the scaling of the magnetoresistance (MR) with the bulk mobility of the OSC as a function of temperature, together with the dependence of the MR on the interlayer thickness, clearly indicates spin injection and transport in TIPS-pentacene. From OSC-spacer thickness-dependent MR measurements, a spin relaxation length of TIPS-pentacene of (24+/-6) nm and a spin relaxation time of approximately 3.5 μs at room temperature are estimated, taking the measured bulk mobility of holes into account.

Adsorption and electronic properties of pentacene on thin dielectric decoupling layers

PubMed Central

Kabakchiev, Alexander; Kuhnke, Klaus; Kern, Klaus

2017-01-01

With the increasing use of thin dielectric decoupling layers to study the electronic properties of organic molecules on metal surfaces, comparative studies are needed in order to generalize findings and formulate practical rules. In this paper we study the adsorption and electronic properties of pentacene deposited onto h-BN/Rh(111) and compare them with those of pentacene deposited onto KCl on various metal surfaces. When deposited onto KCl, the HOMO and LUMO energies of the pentacene molecules scale with the work functions of the combined KCl/metal surface. The magnitude of the variation between the respective KCl/metal systems indicates the degree of interaction of the frontier orbitals with the underlying metal. The results confirm that the so-called IDIS model developed by Willenbockel et al. applies not only to molecular layers on bare metal surfaces, but also to individual molecules on thin electronically decoupling layers. Depositing pentacene onto h-BN/Rh(111) results in significantly different adsorption characteristics, due to the topographic corrugation of the surface as well as the lateral electric fields it presents. These properties are reflected in the divergence from the aforementioned trend for the orbital energies of pentacene deposited onto h-BN/Rh(111), as well as in the different adsorption geometry. Thus, the highly desirable capacity of h-BN to trap molecules comes at the price of enhanced metal–molecule interaction, which decreases the HOMO–LUMO gap of the molecules. In spite of the enhanced interaction, the molecular orbitals are evident in scanning tunnelling spectroscopy (STS) and their shapes can be resolved by spectroscopic mapping. PMID:28900594

Dependence of the Carrier Transport Characteristics on the Buried Layer Thickness in Ambipolar Double-Layer Organic Field-Effect Transistors Investigated by Electrical and Optical Measurements

NASA Astrophysics Data System (ADS)

Zhang, Le; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2013-05-01

By using current-voltage (I-V) measurements and optical modulation spectroscopy, we investigated the dependence of the carrier behaviour on the film thickness of the buried pentacene layer in C60/pentacene ambipolar double-layer organic field-effect transistors (OFETs). It was found that the buried pentacene layer not only acted as a hole transport layer, but also accounted for the properties of the C60/pentacene interface. The hole and electron behaviour exhibited different thickness dependence on the buried pentacene layer, implying the presence of the spatially separated conduction paths. It was suggested that the injected holes transported along the pentacene/gate dielectric interface, which were little affected by the buried pentacene layer thickness or the upper C60 layer; while, the injected electrons accumulated at the C60/pentacene interface, which were sensitive to the interfacial conditions or the buried pentacene layer. Furthermore, it was suggested that the enhanced surface roughness of the buried pentacene layer was responsible for the observed electron behaviour, especially when dpent>10 nm.

Vertical phase separation of 6,13-bis(triisopropylsilylethynyl) pentacene/poly(methyl methacrylate) blends prepared by electrostatic spray deposition for organic field-effect transistors

NASA Astrophysics Data System (ADS)

Onojima, Norio; Hara, Kazuhiro; Nakamura, Ayato

2017-05-01

Blend films composed of 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS pentacene) and poly(methyl methacrylate) (PMMA) were prepared by electrostatic spray deposition (ESD). ESD is considered as an intermediate process between dry and wet processes since the solvent present in small droplets can almost be evaporated before arriving at the substrate. Post-drying treatments with the time-consuming evaporation of residual solvents can be omitted. However, it is still not clear that a vertically phase-separated structure can be formed in the ESD process since the vertical phase separation of the blend films is associated with the solvent evaporation. In this study, we fabricated bottom-gate, top-contact organic field-effect transistors based on the blend films prepared by ESD and the devices exhibited transistor behavior with small hysteresis. This result demonstrates that the vertical phase separation of a blend film (upper TIPS pentacene active layer/bottom PMMA gate insulator) can occur in the facile one-step ESD process.

In situ STM imaging of the structures of pentacene molecules adsorbed on Au(111).

PubMed

Pong, Ifan; Yau, Shuehlin; Huang, Peng-Yi; Chen, Ming-Chou; Hu, Tarng-Shiang; Yang, Yawchia; Lee, Yuh-Lang

2009-09-01

In situ scanning tunneling microscope (STM) was used to examine the spatial structures of pentacene molecules adsorbed onto a Au(111) single-crystal electrode from a benzene dosing solution containing 16-400 microM pentacene. Molecular-resolution STM imaging conducted in 0.1 M HClO(4) revealed highly ordered pentacene structures of ( radical31 x radical31)R8.9 degrees , (3 x 10), ( radical31 x 10), and ( radical7 x 2 radical7)R19.1 degrees adsorbed on the reconstructed Au(111) electrode dosed with different pentacene solutions. These pentacene structures and the reconstructed Au(111) substrate were stable between 0.2 and 0.8 V [vs reversible hydrogen electrode, RHE]. Increasing the potential to E > 0.8 V lifted the reconstructed Au(111) surface and disrupted the ordered pentacene adlattices simultaneously. Ordered pentacene structures could be restored by applying potentials negative enough to reinforce the reconstructed Au(111). At potentials negative of 0.2 V, the adsorption of protons became increasingly important to displace adsorbed pentacene admolecules. Although the reconstructed Au(111) structure was not essential to produce ordered pentacene adlayers, it seemed to help the adsorption of pentacene molecules in a long-range ordered pattern. At room temperature (25 degrees C), approximately 100 pentacene molecules seen in STM images could rotate and align themselves to a neighboring domain in 10 s, suggesting that pentacene admolecules could be mobile on Au(111) under the STM imaging conditions of -150 mV in bias voltage and 1 nA in feedback current.

Nanocomposite Gate Dielectrics With Nanoparticles for Organic Thin Film Transistors

DTIC Science & Technology

2006-09-15

gives rise to the larger transport activation energy and trap distribution width in pentacene TFTs, leading to a decrease of carrier mobility. On the...voltage, carrier mobility of pentacene TFTs increase. These phenomena can be explained by multiple trapping and release model. Therefore, a possible...the low charge carrier mobility of organic semiconductors. Hence, for the applications that require high current output, such as switching of organic

Bandlike Transport in Ferroelectric-Based Organic Field-Effect Transistors

NASA Astrophysics Data System (ADS)

Laudari, A.; Guha, S.

2016-10-01

The dielectric constant of polymer-ferroelectric dielectrics may be tuned by changing the temperature, offering a platform for monitoring changes in interfacial transport with the polarization strength in organic field-effect transistors (FETs). Temperature-dependent transport studies of FETs are carried out from a solution-processed organic semiconductor, 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene), using both ferroelectric- and nonferroelectric-gate insulators. Nonferroelectric dielectric-based TIPS-pentacene FETs show a clear activated transport, in contrast to the ferroelectric dielectric polymer, poly(vinylidene fluoride-trifluoroethylene), where a negative temperature coefficient of the mobility is observed in the ferroelectric temperature range. The current-voltage (I -V ) characteristics from TIPS-pentacene diodes signal a space-charge-limited conduction (SCLC) for a discrete set of trap levels, suggesting that charge injection and transport occurs through regions of ordering in the semiconductor. The carrier mobility extracted from temperature-dependent I -V characteristics from the trap-free SCLC region shows a negative coefficient beyond 200 K, similar to the trend observed in FETs with the ferroelectric dielectric. At moderate temperatures, the polarization-fluctuation-dominant transport inherent in a ferroelectric dielectric, in conjunction with the nature of traps, results in an effective detrapping of the shallow-trap states into more mobile states in TIPS-pentacene.

Inverter Circuits using Pentacene and ZnO Transistors

NASA Astrophysics Data System (ADS)

Iechi, Hiroyuki; Watanabe, Yasuyuki; Kudo, Kazuhiro

2007-04-01

We report two types of integrated circuits based on a pentacene static-induction transistor (SIT), a pentacene thin-film transistor (TFT) and a zinc oxide (ZnO) TFT. The operating characteristics of a p-p inverter using pentacene SITs and a complementary inverter using a p-channel pentacene TFT and an n-channel ZnO TFT are described. The basic operation of logic circuits at a low voltage was achieved for the first time using the pentacene SIT inverter and complementary circuits with hybrid inorganic and organic materials. Furthermore, we describe the electrical properties of the ZnO films depending on sputtering conditions, and the complementary circuits using ZnO and pentacene TFTs.

Low-voltage bendable pentacene thin-film transistor with stainless steel substrate and polystyrene-coated hafnium silicate dielectric.

PubMed

Yun, Dong-Jin; Lee, Seunghyup; Yong, Kijung; Rhee, Shi-Woo

2012-04-01

The hafnium silicate and aluminum oxide high-k dielectrics were deposited on stainless steel substrate using atomic layer deposition process and octadecyltrichlorosilane (OTS) and polystyrene (PS) were treated improve crystallinity of pentacene grown on them. Besides, the effects of the pentacene deposition condition on the morphologies, crystallinities and electrical properties of pentacene were characterized. Therefore, the surface treatment condition on dielectric and pentacene deposition conditions were optimized. The pentacene grown on polystyrene coated high-k dielectric at low deposition rate and temperature (0.2-0.3 Å/s and R.T.) showed the largest grain size (0.8-1.0 μm) and highest crystallinity among pentacenes deposited various deposition conditions, and the pentacene TFT with polystyrene coated high-k dielectric showed excellent device-performance. To decrease threshold voltage of pentacene TFT, the polystyrene-thickness on high-k dielectric was controlled using different concentration of polystyrene solution. As the polystyrene-thickness on hafnium silicate decreases, the dielectric constant of polystyrene/hafnium silicate increases, while the crystallinity of pentacene grown on polystyrene/hafnium silicate did not change. Using low-thickness polystyrene coated hafnium silicate dielectric, the high-performance and low voltage operating (<5 V) pentacene thin film transistor (μ: ~2 cm(2)/(V s), on/off ratio, >1 × 10(4)) and complementary inverter (DC gains, ~20) could be fabricated.

Comprehensive mass spectrometric analysis of novel organic semiconductor molecules

NASA Astrophysics Data System (ADS)

Prada, Svitlana

This work presents a comprehensive mass spectrometry (MS) study of novel organic semiconductor molecules including ion mobility/reactivity measurements and trace elemental analysis. The organic molecules investigated here are important semiconductor materials for molecular electronic devices such as Organic Field-Effect Transistors (OFETs) and Light Emitted Diodes (LED). A high-performance orthogonal time-of flight mass spectrometer (TOF-MS) in combination with a matrix assisted laser desorption/ionization (MALDI) source operating at elevated pressure was used to perform MALDI/TOF analyses of pentacene and some of its derivatives with and without an added matrix. The observation of ion-molecule reactions between "cold" analyte ions and neutral analyte molecules in the gas phase has provided some insight into the mechanism of pentacene cluster formation and its functionalized derivatives. Furthermore, some of the matrices employed to assist the desorption/ionization process of these compounds were observed to influence the outcome via ion-molecule reactions of analyte ions and matrix molecules in the gas phase. The stability and reactivity of the compounds and their clusters in the MALDI plume during gas-phase expansion were evaluated; possible structures of the resulting clusters are discussed. The MALDI/TOF technique was also helpful in distinguishing between two isomeric forms of bis-[(triisopropylsilyl)-ethynyl]-pentacene. Furthermore, we reported ion mobility measurements of functionalized pentacene ions with a modified triple quadrupole mass spectrometer fitted with an ion molecule reactor (IMR). The IMR is equipped with a variable axial electrostatic drift field (ADF) and is able to trap ions for a prolong period of time. These capabilities were successfully employed in the measurement of ion mobilities in different modes of the IMR operation. Theoretical modeling of the drift dynamics and the special localization of the large ion packet was successfully implemented. The contribution of the quadrupole RF field to the drift dynamics also was taken into consideration. The IMR was successfully employed in the ion-molecule reactions study of four functionalized pentacene derivatives such as TIPS, o-TIPS, 6,13-bis-[(triisopropylsilyl)-ethynyl]-pentacene-2,3-dicarbonitrile (TIPS(CN)2), and 6,13-bis-[(triisopropylsilyl)-ethynyl]-pentacene-2,3,9,10-tetracarbonitrile (TIPS(CN)4). Details of the IMR operation in this mode are extensively discussed. The purity of the starting material is one of the most important parameters for the fabrication of a molecular electronic device. We report the method of determination of trace elemental impurities (Li, Na, Al, Mg, Be, Pb, Mn, Co, Ti, Sn, Cu, Cr, V, Zn, Fe, Ca, K and Ni) in organic semiconductor materials, such as Tetracene, Anthracene, Pentacene, TIPS and Rubrene, using an inductively coupled plasma quadrupole mass spectrometer (ICP-MS) fitted with a dynamic reaction cell (DRC). The determination of Fe, Ca, K and Ni in the organic semiconductor materials was carried out using NH3 as a reaction gas in the DRC mode to obviate the effect of polyatomic isobaric interferences. The other trace elements such as Li, Na, Al, Mg, Be, Pb, Mn, Co, Ti, Sn, Cu, Cr, V and Zn have been determined under standard operating conditions.

Effect of multi-dimensional ultraviolet light exposure on the growth of pentacene film and application to organic field-effect transistors.

PubMed

Bae, Jin-Hyuk; Lee, Sin-Doo; Choi, Jong Sun; Park, Jaehoon

2012-05-01

We report on the multi-dimensional alignment of pentacene molecules on a poly(methyl methacrylate)-based photosensitive polymer (PMMA-polymer) and its effect on the electrical performance of the pentacene-based field-effect transistor (FET). Pentacene molecules are shown to be preferentially aligned on the linearly polarized ultraviolet (LPUV)-exposed PMMA-polymer layer, which is contrast to an isotropic alignment on the bare PMMA-polymer layer. Multi-dimensional alignment of pentacene molecules in the film could be achieved by adjusting the direction of LPUV exposed to the PMMA-polymer. The control of pentacene molecular alignment is found to be promising for the field-effect mobility enhancement in the pentacene FET.

Formation of pentacene wetting layer on the SiO2 surface and charge trap in the wetting layer.

PubMed

Kim, Chaeho; Jeon, D

2008-09-01

We studied the early-stage growth of vacuum-evaporated pentacene film on a native SiO(2) surface using atomic force microscopy and in-situ spectroscopic ellipsometry. Pentacene deposition prompted an immediate change in the ellipsometry spectra, but atomic force microscopy images of the early stage films did not show a pentacene-related morphology other than the decrease in the surface roughness. This suggested that a thin pentacene wetting layer was formed by pentacene molecules lying on the surface before the crystalline islands nucleated. Growth simulation based on the in situ spectroscopic ellipsometry spectra supported this conclusion. Scanning capacitance microscopy measurement indicated the existence of trapped charges in the SiO(2) and pentacene wetting layer.

Uniaxial alignment of triisopropylsilylethynyl pentacene via zone-casting technique.

PubMed

Su, Yajun; Gao, Xiang; Liu, Jiangang; Xing, Rubo; Han, Yanchun

2013-09-14

Uniaxially aligned triisopropylsilylethynyl pentacene (TIPS-pentacene) crystals over a large area were fabricated using zone-casting technique. The array of TIPS-pentacene displayed a high orientation degree with a dichroic ratio (DR) of 0.80. The crystals were arranged with c axis perpendicular to the substrate and the long axis of the ribbon corresponded to the a axis of TIPS-pentacene. The properties of the solutions and the processing parameters were shown to influence the formation of the oriented TIPS-pentacene crystalline array. Solvent with a low boiling point (such as chloroform) favoured the orientation of the ribbon-like crystals. The concentration of the solution should be appropriate, ensuring the crystallization velocity of TIPS-pentacene matching with the receding of the meniscus. Besides, we proved that the casting speed should be large enough to induce a sufficient concentration gradient. The orientation mechanism of TIPS-pentacene was attributed to a synergy of the ordered nuclei and a match between the crystallization velocity and the casting speed. Field effect transistors (FETs) based on the oriented TIPS-pentacene crystalline array showed a mobility of 0.67 cm(2) V(-1) s(-1).

Trap-induced photoconductivity in singlet fission pentacene diodes

NASA Astrophysics Data System (ADS)

Qiao, Xianfeng; Zhao, Chen; Chen, Bingbing; Luan, Lin

2014-07-01

This paper reports a trap-induced photoconductivity in ITO/pentacene/Al diodes by using current-voltage and magneto-conductance measurements. The comparison of photoconductivity between pentacene diodes with and without trap clearly shows that the traps play a critical role in generating photoconductivity. It shows that no observable photoconductivity is detected for trap-free pentacene diodes, while significant photoconductivity is observed in diodes with trap. This is because the initial photogenerated singlet excitons in pentacene can rapidly split into triplet excitons with higher binding energy prior to dissociating into free charge carriers. The generated triplet excitons react with trapped charges to release charge-carriers from traps, leading to a trap-induced photoconductivity in the single-layer pentacene diodes. Our studies elucidated the formation mechanisms of photoconductivity in pentacene diodes with extremely fast singlet fission rate.

Interfacial dynamic surface traps of lead sulfide (PbS) nanocrystals: test-platform for interfacial charge carrier traps at the organic/inorganic functional interface

NASA Astrophysics Data System (ADS)

Kim, Youngjun; Ko, Hyungduk; Park, Byoungnam

2018-04-01

Nanocrystal (NC) size and ligand dependent dynamic trap formation of lead sulfide (PbS) NCs in contact with an organic semiconductor were investigated using a pentacene/PbS field effect transistor (FET). We used a bilayer pentacene/PbS FET to extract information of the surface traps of PbS NCs at the pentacene/PbS interface through the field effect-induced charge carrier density measurement in the threshold and subthreshold regions. PbS size and ligand dependent trap properties were elucidated by the time domain and threshold voltage measurements in which threshold voltage shift occurs by carrier charging and discharging in the trap states of PbS NCs. The observed threshold voltage shift is interpreted in context of electron trapping through dynamic trap formation associated with PbS NCs. To the best of our knowledge, this is the first demonstration of the presence of interfacial dynamic trap density of PbS NC in contact with an organic semiconductor (pentacene). We found that the dynamic trap density of the PbS NC is size dependent and the carrier residence time in the specific trap sites is more sensitive to NC size variation than to NC ligand exchange. The probing method presented in the study offers a means to investigate the interfacial surface traps at the organic-inorganic hetero-junction, otherwise understanding of the buried surface traps at the functional interface would be elusive.

Fabrication and Characteristics of Pentacene/Vanadium Pentoxide Field-Effect Transistors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Minagawa, M.; Nakai, K.; Baba, A.

2011-12-23

Organic field-effect transistors (OFETs) were fabricated using pentacene thin layer, and the effects of inserted Lewis-acid thin layers on electrical properties were investigated. The OFETs have active layers of pentacene and vanadium pentoxide (V{sub 2}O{sub 5}) as a Lewis-acid layer. Typical source-drain current (I{sub DS}) vs. source-drain voltage (V{sub DS}) curves were observed under negative gate voltages (V{sub G}S) application, and the shift of the threshold voltage for FET driving (V{sub t}) to positive side was also observed by V{sub 2}O{sub 5} layer insertion, that is, -2.5 V for device with V{sub 2}O{sub 5} layer and -5.7 V for devicemore » without V{sub 2}O{sub 5} layer. It was thought that charge transfer (CT) complexes which were formed at the interface between pentacene and V{sub 2}O{sub 5} layer were dissociated by the applied gate voltage, and the generated holes seem to contribute to drain current and the apparent V{sub t} improvement.« less

Template-Assisted Benzannulation Route to Pentacene and Tetracene Derivatives and its Application to Construct Amphiphilic Acenes That Self-Assemble into Helical Wires.

PubMed

Pal, Bikash; Chang, Chun-Hsiung; Zeng, Cian-Jhe; Lin, Chih-Hsiu

2017-12-11

Pentacene is one of the most versatile organic semiconductors. New synthetic strategies to construct the pentacene skeleton are imperative to produce pentacene derivatives with appropriate solubility, stability, and optoelectronic properties for various applications. This paper describes a template-directed approach to pentacene derivatives. In the retrosynthesis, the acene skeleton is viewed as a laddered double strand polyene instead of the more intuitive linearly fused hexagons. Based on this vision, the template strand of polyene is constructed with Wittig olefination, whereas the second strand is accomplished with Knoevenagel condensation to produce pentacene and tetracene derivatives. The synthetic scheme is flexible enough to generate an array of acene derivatives with substitution patterns that were hitherto difficult to access. Amphiphilic pentacene and tetracene derivatives were also synthesized by the template strategy. One pentacene based amphiphilic rod-coil molecule undergoes self-assembly to form helical wire structures that were visualized with TEM. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Structural properties 3,16-bis triisopropylsilylethynyl (pentacene) (TIPS-pentacene) thin films onto organic dielectric layer using slide coating method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rusnan, Fara Naila; Mohamad, Khairul Anuar; Seria, Dzul Fahmi Mohd Husin

3,16-bis triisopropylsilylethynyl (Pentacene) (TIPS-Pentacene) compactable interface property is important in order to have a good arrangement of molecular structure. Comparison for TIPS-Pentacene deposited between two different surface layers conducted. 0.1wt% TIPS-Pentacene diluted in chloroform were deposited onto poly(methylmeaclyrate) (PMMA) layered transparent substrates using slide coating method. X-ray diffraction (XRD) used to determine crystallinity of thin films. Series of (00l) diffraction peaks obtained with sharp first peaks (001) for TIPS-Pentacene deposited onto PMMA layer at 5.35° and separation of 16.3 Å. Morphology and surface roughness were carried out using scanning electron microscope (SEM) and surface profilemeter LS500, respectively.TIPS-Pentacene deposited onto PMMAmore » layer formed needled-like-shape grains with 10.26 nm surface roughness. These properties were related as thin film formed and its surface roughness plays important role towards good mobility devices.« less

Effect of dielectric layers on device stability of pentacene-based field-effect transistors.

PubMed

Di, Chong-an; Yu, Gui; Liu, Yunqi; Guo, Yunlong; Sun, Xiangnan; Zheng, Jian; Wen, Yugeng; Wang, Ying; Wu, Weiping; Zhu, Daoben

2009-09-07

We report stable organic field-effect transistors (OFETs) based on pentacene. It was found that device stability strongly depends on the dielectric layer. Pentacene thin-film transistors based on the bare or polystyrene-modified SiO(2) gate dielectrics exhibit excellent electrical stabilities. In contrast, the devices with the octadecyltrichlorosilane (OTS)-treated SiO(2) dielectric layer showed the worst stabilities. The effects of the different dielectrics on the device stabilities were investigated. We found that the surface energy of the gate dielectric plays a crucial role in determining the stability of the pentacene thin film, device performance and degradation of electrical properties. Pentacene aggregation, phase transfer and film morphology are also important factors that influence the device stability of pentacene devices. As a result of the surface energy mismatch between the dielectric layer and organic semiconductor, the electronic performance was degraded. Moreover, when pentacene was deposited on the OTS-treated SiO(2) dielectric layer with very low surface energy, pentacene aggregation occurred and resulted in a dramatic decrease of device performance. These results demonstrated that the stable OFETs could be obtained by using pentacene as a semiconductor layer.

Face-to-Face Packing of 2,3,9,10-Tetrasubstituted Pentacene Derivatives Revealed through a Solid State [4 + 4] Thermal Cycloaddition and Molecular Dynamic Simulation.

PubMed

Pal, Bikash; Lin, Bo-Chao; Dela Cerna, Mark Vincent Carreon; Hsu, Chao-Ping; Lin, Chih-Hsiu

2016-08-05

2,3,9,10-Substituted pentacene tetraesters and pentacene diester-dinitriles were synthesized. These pentacene derivatives underwent an unusual solid state [4 + 4] thermal dimerization with good efficiency and complete stereoselectivity. This observation indicates this series of pentacene derivatives adopt π-π stacking geometry with large mutual overlap in solid state. This notion was confirmed by molecualr dynamic simulation.

Current transport across the pentacene/CVD-grown graphene interface for diode applications.

PubMed

Berke, K; Tongay, S; McCarthy, M A; Rinzler, A G; Appleton, B R; Hebard, A F

2012-06-27

We investigate the electronic transport properties across the pentacene/graphene interface. Current transport across the pentacene/graphene interface is found to be strikingly different from transport across pentacene/HOPG and pentacene/Cu interfaces. At low voltages, diodes using graphene as a bottom electrode display Poole–Frenkel emission, while diodes with HOPG and Cu electrodes are dominated by thermionic emission. At high voltages conduction is dominated by Poole–Frenkel emission for all three junctions. We propose that current across these interfaces can be accurately modeled by a combination of thermionic and Poole–Frenkel emission. Results presented not only suggest that graphene provides low resistive contacts to pentacene where a flat-laying orientation of pentacene and transparent metal electrodes are desired but also provides further understanding of the physics at the organic semiconductor/graphene interface.

Resistive switching behaviors of Au/pentacene/Si-nanowire arrays/heavily doped n-type Si devices for memory applications

NASA Astrophysics Data System (ADS)

Tsao, Hou-Yen; Lin, Yow-Jon

2014-02-01

The fabrication of memory devices based on the Au/pentacene/heavily doped n-type Si (n+-Si), Au/pentacene/Si nanowires (SiNWs)/n+-Si, and Au/pentacene/H2O2-treated SiNWs/n+-Si structures and their resistive switching characteristics were reported. A pentacene memory structure using SiNW arrays as charge storage nodes was demonstrated. The Au/pentacene/SiNWs/n+-Si devices show hysteresis behavior. H2O2 treatment may lead to the hysteresis degradation. However, no hysteresis-type current-voltage characteristics were observed for Au/pentacene/n+-Si devices, indicating that the resistive switching characteristic is sensitive to SiNWs and the charge trapping effect originates from SiNWs. The concept of nanowires within the organic layer opens a promising direction for organic memory devices.

The role of charge transfer in the energy level alignment at the pentacene/C60 interface.

PubMed

Beltrán, J; Flores, F; Ortega, J

2014-03-07

Understanding the mechanism of energy level alignment at organic-organic interfaces is a crucial line of research to optimize applications in organic electronics. We address this problem for the C60-pentacene interface by performing local-orbital Density Functional Theory (DFT) calculations, including the effect of the charging energies on the energy gap of both organic materials. The results are analyzed within the induced density of interface states (IDIS) model. We find that the induced interface potential is in the range of 0.06-0.10 eV, in good agreement with the experimental evidence, and that such potential is mainly induced by the small, but non-negligible, charge transfer between the two compounds and the multipolar contribution associated with pentacene. We also suggest that an appropriate external intercompound potential could create an insulator-metal transition at the interface.

Effect of dynamic disorder on charge transport along a pentacene chain

NASA Astrophysics Data System (ADS)

Böhlin, J.; Linares, M.; Stafström, S.

2011-02-01

The lattice equation of motion and a numerical solution of the time-dependent Schrödinger equation provide us with a microscopic picture of charge transport in highly ordered molecular crystals. We have chosen the pentacene single crystal as a model system, and we study charge transport as a function of phonon-mode time-dependent fluctuations in the intermolecular electron transfer integral. For comparison, we include similar fluctuations also in the intramolecular potentials. The variance in these energy quantities is closely related to the temperature of the system. The pentacene system is shown to be very sensitive to fluctuation in the intermolecular transfer integral, revealing a transition from adiabatic to nonadiabatic polaron transport for increasing temperatures. The extension of the polaron at temperatures above 200 K is limited by the electron localization length rather than the interplay between the electron transfer integral and the electron-phonon coupling strength.

Graphene quantum dot (GQD)-induced photovoltaic and photoelectric memory elements in a pentacene/GQD field effect transistor as a probe of functional interface

NASA Astrophysics Data System (ADS)

Kim, Youngjun; Cho, Seongeun; Kim, Hyeran; Seo, Soonjoo; Lee, Hyun Uk; Lee, Jouhahn; Ko, Hyungduk; Chang, Mincheol; Park, Byoungnam

2017-09-01

Electric field-induced charge trapping and exciton dissociation were demonstrated at a penatcene/grapheme quantum dot (GQD) interface using a bottom contact bi-layer field effect transistor (FET) as an electrical nano-probe. Large threshold voltage shift in a pentacene/GQD FET in the dark arises from field-induced carrier trapping in the GQD layer or GQD-induced trap states at the pentacene/GQD interface. As the gate electric field increases, hysteresis characterized by the threshold voltage shift depending on the direction of the gate voltage scan becomes stronger due to carrier trapping associated with the presence of a GQD layer. Upon illumination, exciton dissociation and gate electric field-induced charge trapping simultaneously contribute to increase the threshold voltage window, which can potentially be exploited for photoelectric memory and/or photovoltaic devices through interface engineering.

Insertion of a pentacene layer into the gold/poly(methyl methacrylate)/heavily doped p-type Si/indium device leading to the modulation of resistive switching characteristics

NASA Astrophysics Data System (ADS)

Hung, Cheng-Chun; Lin, Yow-Jon

2018-01-01

In order to get a physical insight into the pentacene interlayer-modulated resistive switching (RS) characteristics, the Au/pentacene/poly(methyl methacrylate) (PMMA)/heavily doped p-type Si (p+-Si)/In and Au/PMMA/p+-Si/In devices are fabricated and the device performance is provided. The Au/pentacene/PMMA/p+-Si/In device shows RS behavior, whereas the Au/PMMA/p+-Si/In device exhibits the set/reset-free hysteresis current-voltage characteristics. The insertion of a pentacene layer is a noticeable contribution to the RS characteristic. This is because of the occurrence of carrier accumulation/depletion in the pentacene interlayer. The transition from carrier depletion to carrier accumulation (carrier accumulation to carrier depletion) in pentacene occurring under negative (positive) voltage induces the process of set (reset). The switching conduction mechanism is primarily described as space charge limited conduction according to the electrical transport properties measurement. The concept of a pentacene/PMMA heterostructure opens a promising direction for organic memory devices.

Computationally derived rules for persistence of C60 nanowires on recumbent pentacene bilayers.

PubMed

Cantrell, Rebecca A; James, Christine; Clancy, Paulette

2011-08-16

The tendency for C(60) nanowires to persist on two monolayers of recumbent pentacene is studied using molecular dynamics (MD) simulations. A review of existing experimental literature for the tilt angle adopted by pentacene on noble metal surfaces shows that studies cover a limited range from 55° to 90°, motivating simulation studies of essentially the entire range of tilt angles (10°-90°) to predict the optimum surface tilt angle for C(60) nanowire formation. The persistence of a 1D nanowire depends sensitively on this tilt angle, the amount of initial tensile strain, and the presence of surface step edges. At room temperature, C(60) nanowires oriented along the pentacene short axes persist for several nanoseconds and are more likely to occur if they reside between, or within, pentacene rows for ϕ ≤ ∼60°. The likelihood of this persistence increases the smaller the tilt angle. Nanowires oriented along the long axes of pentacene molecules are unlikely to form. The limit of stability of nanowires was tested by raising the temperature to 400 K. Nanowires located between pentacene rows survived this temperature rise, but those located initially within pentacene rows are only stable in the range ϕ(1) = 30°-50°. Flatter pentacene surfaces, that is, tilt angles above about 60°, are subject to disorder caused by C(60) molecules "burrowing" into the pentacene surface. An initial strain of 5% applied to the C(60) nanowires significantly decreases the likelihood of nanowire persistence. In contrast, any appreciable surface roughness, even by half a monolayer in height of a third pentacene monolayer, strongly enhances the likelihood of nanowire formation due to the strong binding energy of C(60) molecules to step edges.

Improved organic thin-film transistor performance using novel self-assembled monolayers

NASA Astrophysics Data System (ADS)

McDowell, M.; Hill, I. G.; McDermott, J. E.; Bernasek, S. L.; Schwartz, J.

2006-02-01

Pentacene-based organic thin-film transistors have been fabricated using a phosphonate-linked anthracene self-assembled monolayer as a buffer between the silicon dioxide gate dielectric and the active pentacene channel region. Vast improvements in the subthreshold slope and threshold voltage are observed compared to control devices fabricated without the buffer. Both observations are consistent with a greatly reduced density of charge trapping states at the semiconductor-dielectric interface effected by introduction of the self-assembled monolayer.

N-Heterocyclic-Carbene-Treated Gold Surfaces in Pentacene Organic Field-Effect Transistors: Improved Stability and Contact at the Interface.

PubMed

Lv, Aifeng; Freitag, Matthias; Chepiga, Kathryn M; Schäfer, Andreas H; Glorius, Frank; Chi, Lifeng

2018-04-16

N-Heterocyclic carbenes (NHCs), which react with the surface of Au electrodes, have been successfully applied in pentacene transistors. With the application of NHCs, the charge-carrier mobility of pentacene transistors increased by five times, while the contact resistance at the pentacene-Au interface was reduced by 85 %. Even after annealing the NHC-Au electrodes at 200 °C for 2 h before pentacene deposition, the charge-carrier mobility of the pentacene transistors did not decrease. The distinguished performance makes NHCs as excellent alternatives to thiols as metal modifiers for the application in organic field-effect transistors (OFETs). © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Interface characteristics at an organic/metal junction: pentacene on Cu stepped surfaces.

PubMed

Matos, Jeronimo; Kara, Abdelkader

2016-11-09

The adsorption of pentacene on Cu (2 2 1), Cu (5 1 1) and Cu (9 1 1) is investigated using density functional theory (DFT) with the self-consistent inclusion of van der Waals (vdW) interactions. Cu (2 1 1) is a vicinal of Cu (1 1 1) while Cu (5 1 1) and (9 1 1) are vicinals of Cu (1 0 0). For all the three surfaces, we found pentacene to prefer to adsorb parallel to the surface and near the steps. The addition of vdW interactions resulted in an enhancement in adsorption energies, with reference to the PBE functional, of around 2 eV. With vdWs inclusion, the adsorption energies were found to be 2.98 eV, 3.20 eV and 3.49 eV for Cu (2 2 1), Cu (5 1 1) and Cu (9 1 1) respectively. These values reflect that pentacene adsorbs stronger on (1 0 0) terraces with a preference for larger terraces. The molecule tilts upon adsorption with a small tilt angle on the (1 0 0) vicinals (about a few degrees) as compared to a large one on Cu (2 2 1) where the tilt angle is found to be about 20°. We find that the adsorption results in a net charge transfer to the molecule of ~1 electron, for all surfaces.

Ion-mobility study of two functionalized pentacene structural isomers using a modified electrospray/triple quadrupole mass spectrometer

NASA Astrophysics Data System (ADS)

Prada, Svitlana V.; Bohme, Diethard K.; Baranov, Vladimir I.

2007-03-01

We report ion-mobility measurements with a modified triple quadrupole mass spectrometer fitted with an ion molecule reactor (IMR) designed to investigate ion molecule reactivity in organic mass spectrometry. Functionalized pentacene ions, which are generally unreactive were chosen for study to decouple drift/diffusion effects from reactivity (including clustering). The IMR is equipped with a variable axial electrostatic drift field (ADF) and is able to trap ions. These capabilities were successfully employed in the measurement of ion mobilities in different modes of IMR operation. Theoretical modeling of the drift dynamics and the special localization of the large ion packet was successfully implemented. The contribution of the quadrupole RF field to the drift dynamics also was taken into consideration.

Effect of nanocomposite gate-dielectric properties on pentacene microstructure and field-effect transistor characteristics.

PubMed

Lee, Wen-Hsi; Wang, Chun-Chieh

2010-02-01

In this study, the effect of surface energy and roughness of the nanocomposite gate dielectric on pentacene morphology and electrical properties of pentacene OTFT are reported. Nanoparticles TiO2 were added in the polyimide matrix to form a nanocomposite which has a significantly different surface characteristic from polyimide, leading to a discrepancy in the structural properties of pentacene growth. A growth mode of pentacene deposited on the nanocomposite is proposed to explain successfully the effect of surface properties of nanocomposite gate dielectric such as surface energy and roughness on the pentacene morphology and electrical properties of OTFT. To obtain the lower surface energy and smoother surface of nanocomposite gate dielectric that is responsible for the desired crystalline, microstructure of pentacene and electrical properties of device, a bottom contact OTFT-pentacene deposited on the double-layer nanocomposite gate dielectric consisting of top smoothing layer of the neat polyimide and bottom layer of (PI+ nano-TiO2 particles) nanocomposite has been successfully demonstrated to exhibit very promising performance including high current on to off ratio of about 6 x 10(5), threshold voltage of -10 V and moderately high filed mobility of 0.15 cm2V(-1)s(-1).

C60-pentacene network formation by 2-D co-crystallization.

PubMed

Jin, Wei; Dougherty, Daniel B; Cullen, William G; Robey, Steven; Reutt-Robey, Janice E

2009-09-01

We report experiments highlighting the mechanistic role of mobile pentacene precursors in the formation of a network C(60)-pentacene co-crystalline structure on Ag(111). This co-crystalline arrangement was first observed by low temperature scanning tunneling microscopy (STM) by Zhang et al. (Zhang, H. L.; Chen, W.; Huang, H.; Chen, L.; Wee, A. T. S. J. Am. Chem. Soc. 2008, 130, 2720-2721). We now show that this structure forms readily at room temperature from a two-dimensional (2-D) mixture. Pentacene, evaporated onto Ag(111) to coverages of 0.4-1.0 ML, produces a two-dimensional (2-D) gas. Subsequently deposited C(60) molecules combine with the pentacene 2-D gas to generate a network structure, consisting of chains of close-packed C(60) molecules, spaced by individual C(60) linkers and 1 nm x 2.5 nm pores containing individual pentacene molecules. Spontaneous formation of this stoichiometric (C(60))(4)-pentacene network from a range of excess pentacene surface coverage (0.4 to 1.0 ML) indicates a self-limiting assembly process. We refine the structure model for this phase and discuss the generality of this co-crystallization mechanism.

Ambipolar pentacene field-effect transistor with double-layer organic insulator

NASA Astrophysics Data System (ADS)

Kwak, Jeong-Hun; Baek, Heume-Il; Lee, Changhee

2006-08-01

Ambipolar conduction in organic field-effect transistor is very important feature to achieve organic CMOS circuitry. We fabricated an ambipolar pentacene field-effect transistors consisted of gold source-drain electrodes and double-layered PMMA (Polymethylmethacrylate) / PVA (Polyvinyl Alcohol) organic insulator on the ITO(Indium-tin-oxide)-patterned glass substrate. These top-contact geometry field-effect transistors were fabricated in the vacuum of 10 -6 Torr and minimally exposed to atmosphere before its measurement and characterized in the vacuum condition. Our device showed reasonable p-type characteristics of field-effect hole mobility of 0.2-0.9 cm2/Vs and the current ON/OFF ratio of about 10 6 compared to prior reports with similar configurations. For the n-type characteristics, field-effect electron mobility of 0.004-0.008 cm2/Vs and the current ON/OFF ratio of about 10 3 were measured, which is relatively high performance for the n-type conduction of pentacene field-effect transistors. We attributed these ambipolar properties mainly to the hydroxyl-free PMMA insulator interface with the pentacene active layer. In addition, an increased insulator capacitance due to double-layer insulator structure with high-k PVA layer also helped us to observe relatively good n-type characteristics.

C70/C70:pentacene/pentacene organic heterojunction as the connecting layer for high performance tandem organic light-emitting diodes: Mechanism investigation of electron injection and transport

NASA Astrophysics Data System (ADS)

Guo, Qingxun; Yang, Dezhi; Chen, Jiangshan; Qiao, Xianfeng; Ahamad, Tansir; Alshehri, Saad M.; Ma, Dongge

2017-03-01

A high performance tandem organic light-emitting diode (OLED) is realized by employing a C70/C70:pentacene/pentacene organic heterojunction as the efficient charge generation layer (CGL). Not only more than two time enhancement of external quantum efficiency but also significant improvement in both power efficiency and lifetime are well achieved. The mechanism investigations find that the electron injection from the CGL to the adjacent electron transport layer (ETL) in tandem devices is injection rate-limited due to the high interface energy barrier between the CGL and the ETL. By the capacitance-frequency (C-F) and low temperature current density-voltage (J-V) characteristic analysis, we confirm that the electron transport is a space-charge-limited current process with exponential trap distribution. These traps are localized states below the lowest unoccupied molecular orbital edge inside the gap and would be filled with the upward shift of the Fermi level during the n-doping process. Furthermore, both the trap density (Ht) and the activation energy (Ea) could be carefully worked out through low temperature J-V measurements, which is very important for developing high performance tandem OLEDs.

High-Performance Nonvolatile Organic Field-Effect Transistor Memory Based on Organic Semiconductor Heterostructures of Pentacene/P13/Pentacene as Both Charge Transport and Trapping Layers.

PubMed

Li, Wen; Guo, Fengning; Ling, Haifeng; Zhang, Peng; Yi, Mingdong; Wang, Laiyuan; Wu, Dequn; Xie, Linghai; Huang, Wei

2017-08-01

Nonvolatile organic field-effect transistor (OFET) memory devices based on pentacene/ N , N '-ditridecylperylene-3,4,9,10-tetracarboxylic diimide (P13)/pentacene trilayer organic heterostructures have been proposed. The discontinuous n-type P13 embedded in p-type pentacene layers can not only provide electrons in the semiconductor layer that facilitates electron trapping process; it also works as charge trapping sites, which is attributed to the quantum well-like pentacene/P13/pentacene organic heterostructures. The synergistic effects of charge trapping in the discontinuous P13 and the charge-trapping property of the poly(4-vinylphenol) (PVP) layer remarkably improve the memory performance. In addition, the trilayer organic heterostructures have also been successfully applied to multilevel and flexible nonvolatile memory devices. The results provide a novel design strategy to achieve high-performance nonvolatile OFET memory devices and allow potential applications for different combinations of various organic semiconductor materials in OFET memory.

High‐Performance Nonvolatile Organic Field‐Effect Transistor Memory Based on Organic Semiconductor Heterostructures of Pentacene/P13/Pentacene as Both Charge Transport and Trapping Layers

PubMed Central

Li, Wen; Guo, Fengning; Ling, Haifeng; Zhang, Peng; Wang, Laiyuan; Wu, Dequn

2017-01-01

Nonvolatile organic field‐effect transistor (OFET) memory devices based on pentacene/N,N′‐ditridecylperylene‐3,4,9,10‐tetracarboxylic diimide (P13)/pentacene trilayer organic heterostructures have been proposed. The discontinuous n‐type P13 embedded in p‐type pentacene layers can not only provide electrons in the semiconductor layer that facilitates electron trapping process; it also works as charge trapping sites, which is attributed to the quantum well‐like pentacene/P13/pentacene organic heterostructures. The synergistic effects of charge trapping in the discontinuous P13 and the charge‐trapping property of the poly(4‐vinylphenol) (PVP) layer remarkably improve the memory performance. In addition, the trilayer organic heterostructures have also been successfully applied to multilevel and flexible nonvolatile memory devices. The results provide a novel design strategy to achieve high‐performance nonvolatile OFET memory devices and allow potential applications for different combinations of various organic semiconductor materials in OFET memory. PMID:28852619

Direct measurement of density of states in pentacene thin film transistors

NASA Astrophysics Data System (ADS)

Yogev, S.; Halpern, E.; Matsubara, R.; Nakamura, M.; Rosenwaks, Y.

2011-10-01

We report on direct high lateral resolution measurements of density of states in pentacene thin film transistors using Kelvin probe force microscopy. The measurements were conducted on passivated (hexamethyldisilazane) and unpassivated field effect transistors with 10- and 30-nm-thick pentacene polycrystalline layers. The analysis takes into account both the band bending in the organic film and the trapped charge at the SiO2-pentacene interface. We found that the density of states for the highest occupied molecular orbital band of pentacene film on the treated substrate is Gaussian with a width (variance) of σ=0.07±0.01eV and an exponential tail. The concentration of the density of states in the gap for pentacene on bare SiO2 substrate was larger by one order of magnitude, had a different energy distribution, and induced Fermi level pinning. The results are discussed in view of their effect on pentacene thin film transistors’ performance.

Contact effects analyzed by a parameter extraction method based on a single bottom-gate/top-contact organic thin-film transistor

NASA Astrophysics Data System (ADS)

Takagaki, Shunsuke; Yamada, Hirofumi; Noda, Kei

2018-03-01

Contact effects in organic thin-film transistors (OTFTs) were examined by using our previously proposed parameter extraction method from the electrical characteristics of a single staggered-type device. Gate-voltage-dependent contact resistance and channel mobility in the linear regime were evaluated for bottom-gate/top-contact (BGTC) pentacene TFTs with active layers of different thicknesses, and for pentacene TFTs with contact-doped layers prepared by coevaporation of pentacene and tetrafluorotetracyanoquinodimethane (F4TCNQ). The extracted parameters suggested that the influence of the contact resistance becomes more prominent with the larger active-layer thickness, and that contact-doping experiments give rise to a drastic decrease in the contact resistance and a concurrent considerable improvement in the channel mobility. Additionally, the estimated energy distributions of trap density in the transistor channel probably reflect the trap filling with charge carriers injected into the channel regions. The analysis results in this study confirm the effectiveness of our proposed method, with which we can investigate contact effects and circumvent the influences of characteristic variations in OTFT fabrication.

An improved synthesis of pentacene: rapid access to a benchmark organic semiconductor.

PubMed

Pramanik, Chandrani; Miller, Glen P

2012-04-20

Pentacene is an organic semiconductor used in a variety of thin-film organic electronic devices. Although at least six separate syntheses of pentacene are known (two from dihydropentacenes, two from 6,13-pentacenedione and two from 6,13-dihydro-6,13-dihydroxypentacene), none is ideal and several utilize elevated temperatures that may facilitate the oxidation of pentacene as it is produced. Here, we present a fast (-2 min of reaction time), simple, high-yielding (≥ 90%), low temperature synthesis of pentacene from readily available 6,13-dihydro-6,13-dihydroxypentacene. Further, we discuss the mechanism of this highly efficient reaction. With this improved synthesis, researchers gain rapid, affordable access to high purity pentacene in excellent yield and without the need for a time consuming sublimation.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Qiao, Xianfeng, E-mail: qiaoxianfeng@hotmail.com; Zhao, Chen; Chen, Bingbing

This paper reports a trap-induced photoconductivity in ITO/pentacene/Al diodes by using current-voltage and magneto-conductance measurements. The comparison of photoconductivity between pentacene diodes with and without trap clearly shows that the traps play a critical role in generating photoconductivity. It shows that no observable photoconductivity is detected for trap-free pentacene diodes, while significant photoconductivity is observed in diodes with trap. This is because the initial photogenerated singlet excitons in pentacene can rapidly split into triplet excitons with higher binding energy prior to dissociating into free charge carriers. The generated triplet excitons react with trapped charges to release charge-carriers from traps, leadingmore » to a trap-induced photoconductivity in the single-layer pentacene diodes. Our studies elucidated the formation mechanisms of photoconductivity in pentacene diodes with extremely fast singlet fission rate.« less

Carrier mobility in mesoscale heterogeneous organic materials: Effects of crystallinity and anisotropy on efficient charge transport

NASA Astrophysics Data System (ADS)

Kobayashi, Hajime; Shirasawa, Raku; Nakamoto, Mitsunori; Hattori, Shinnosuke; Tomiya, Shigetaka

2017-07-01

Charge transport in the mesoscale bulk heterojunctions (BHJs) of organic photovoltaic devices (OPVs) is studied using multiscale simulations in combination with molecular dynamics, the density functional theory, the molecular-level kinetic Monte Carlo (kMC) method, and the coarse-grained kMC method, which was developed to estimate mesoscale carrier mobility. The effects of the degree of crystallinity and the anisotropy of the conductivity of donors on hole mobility are studied for BHJ structures that consist of crystalline and amorphous pentacene grains that act as donors and amorphous C60 grains that act as acceptors. We find that the hole mobility varies dramatically with the degree of crystallinity of pentacene because it is largely restricted by a low-mobility amorphous region that occurs in the hole transport network. It was also found that the percolation threshold of crystalline pentacene is relatively high at approximately 0.6. This high percolation threshold is attributed to the 2D-like conductivity of crystalline pentacene, and the threshold is greatly improved to a value of approximately 0.3 using 3D-like conductive donors. We propose essential guidelines to show that it is critical to increase the degree of crystallinity and develop 3D conductive donors for efficient hole transport through percolative networks in the BHJs of OPVs.

Space Environment Effects on Flexible, Low-Voltage Organic Thin-Film Transistors.

PubMed

Basiricò, Laura; Basile, Alberto Francesco; Cosseddu, Piero; Gerardin, Simone; Cramer, Tobias; Bagatin, Marta; Ciavatti, Andrea; Paccagnella, Alessandro; Bonfiglio, Annalisa; Fraboni, Beatrice

2017-10-11

Organic electronic devices fabricated on flexible substrates are promising candidates for applications in environments where flexible, lightweight, and radiation hard materials are required. In this work, device parameters such as threshold voltage, charge mobility, and trap density of 13-bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene)-based organic thin-film transistors (OTFTs) have been monitored for performing electrical measurements before and after irradiation by high-energy protons. The observed reduction of charge carrier mobility following irradiation can be only partially ascribed to the increased trap density. Indeed, we used other techniques to identify additional effects induced by proton irradiation in such devices. Atomic force microscopy reveals morphological defects occurring in the organic dielectric layer induced by the impinging protons, which, in turn, induce a strain on the TIPS-pentacene crystallites lying above. The effects of this strain are investigated by density functional theory simulations of two model structures, which describe the TIPS-pentacene crystalline films at equilibrium and under strain. The two different density of states distributions in the valence band have been correlated with the photocurrent spectra acquired before and after proton irradiation. We conclude that the degradation of the dielectric layer and the organic semiconductor sensitivity to strain are the two main phenomena responsible for the reduction of OTFT mobility after proton irradiation.

Enhanced photovoltaic performance in nanoimprinted pentacene-PbS nanocrystal hybrid device

NASA Astrophysics Data System (ADS)

Dissanayake, D. M. N. M.; Adikaari, A. A. D. T.; Silva, S. R. P.

2008-03-01

Pentacene and PbS nanocrystal bilayer photovoltaic devices are fabricated after the pentacene layer is subjected to nanoimprinting using a laser textured silicon stamp. Increased short circuit current densities are observed for the imprinted devices, which are attributed to increased charge mobility in the pentacene film caused by the decrease in the intermolecular distances during nanoimprinting. This work is consistent with previous reports where hydrostatic pressure induced mobility increases have been observed in polyacenes under gigapascal pressure regimes. It is believed that the pentacene film undergoes localized high pressures during nanoimprinting, giving rise to the increased hole mobilities.

Chemical Defects and Electronics States in Organic Semiconductors

DTIC Science & Technology

2008-05-31

from interacting with organic semiconductor devices. An expt./theoretical study of 0 2 in pentacene indicated that a positive gate voltage can cause...dissociative interaction of02 with pentacene . 1S. SUBJECT TERMS organic semiconductors, PBTIT, P3HT, PQT, polythiophenes, pentacene , defects...investigations of the interaction of02 molecules with pentacene were performed. Based on calculations of formation energies of charged defects a model was

Photostability enhancement of the pentacene derivative having two nitronyl nitroxide radical substituents.

PubMed

Shimizu, Akihiro; Ito, Akitaka; Teki, Yoshio

2016-02-18

Pentacene derivatives possessing nitronyl nitroxide radical substituents (1a and 1b) were synthesized, and their photochemical properties were evaluated. 1a with two radical substituents showed a remarkable enhancement of photostability compared with pentacene, 6,13-bis(triisopropylsilylethynyl)pentacene and the monoradical, 1b. This is understood due to the presence of the multiple deactivation pathways in the photoexcited states.

Observation of Spectral Diffusion in Crystals Using Single Impurity Molecules

DTIC Science & Technology

1990-10-31

from 12pentacene photophysical parameters including intersystem crossing . Apparently (and not surprisingly), the local pentacene environment this... pentacene molecules inp-terphenyl, both stable as well as spectrally diffusing single molecules can be observed. 20 DISTRIBUTION/AVAILABILITY OF ABSTRACT 121...with ultrathin sublimed crystals have removed this obstacle. For the case of pentacene impurities in crystals of p-terphenyl, we observe two radically

Percolative effects on noise in pentacene transistors

NASA Astrophysics Data System (ADS)

Conrad, B. R.; Cullen, W. G.; Yan, W.; Williams, E. D.

2007-12-01

Noise in pentacene thin film transistors has been measured as a function of device thickness from well above the effective conduction channel thickness to only two conducting layers. Over the entire thickness range, the spectral noise form is 1/f, and the noise parameter varies inversely with gate voltage, confirming that the noise is due to mobility fluctuations, even in the thinnest films. Hooge's parameter varies as an inverse power law with conductivity for all film thicknesses. The magnitude and transport characteristics of the spectral noise are well explained in terms of percolative effects arising from the grain boundary structure.

Vacancy effects on the electronic and structural properties pentacene

NASA Astrophysics Data System (ADS)

Laraib, Iflah; Janotti, Anderson

Defects in organic crystals are likely to affect charge transport in organic electronic devices. Vacancies can create lattice distortions and modify electronic states associated with the molecules in its surrounding. Spectroscopy experiments indicate that molecular vacancies trap charge carriers. Experimental characterization of individual defects is challenging and unambiguous. Here we use density functional calculations including van der Waals interactions in a supercell approach to study the single vacancy in pentacene, a prototype organic semiconductor. We determine formation energies, local lattice relaxations, and discuss how vacancies locally distort the lattice and affect the electronic properties of the host organic semiconductor.

Field-induced charge transport at the surface of pentacene single crystals: A method to study charge dynamics of two-dimensional electron systems in organic crystals

NASA Astrophysics Data System (ADS)

Takeya, J.; Goldmann, C.; Haas, S.; Pernstich, K. P.; Ketterer, B.; Batlogg, B.

2003-11-01

A method has been developed to inject mobile charges at the surface of organic molecular crystals, and the dc transport of field-induced holes has been measured at the surface of pentacene single crystals. To minimize damage to the soft and fragile surface, the crystals are attached to a prefabricated substrate which incorporates a gate dielectric (SiO2) and four probe pads. The surface mobility of the pentacene crystals ranges from 0.1 to 0.5 cm2/V s and is nearly temperature independent above ˜150 K, while it becomes thermally activated at lower temperatures when the induced charges become localized. Ruling out the influence of electric contacts and crystal grain boundaries, the results contribute to the microscopic understanding of trapping and detrapping mechanisms in organic molecular crystals.

High mobility organic field-effect transistor based on water-soluble deoxyribonucleic acid via spray coating

NASA Astrophysics Data System (ADS)

Shi, Wei; Han, Shijiao; Huang, Wei; Yu, Junsheng

2015-01-01

High mobility organic field-effect transistors (OFETs) by inserting water-soluble deoxyribonucleic acid (DNA) buffer layer between electrodes and pentacene film through spray coating process were fabricated. Compared with the OFETs incorporated with DNA in the conventional organic solvents of ethanol and methanol: water mixture, the water-soluble DNA based OFET exhibited an over four folds enhancement of field-effect mobility from 0.035 to 0.153 cm2/Vs. By characterizing the surface morphology and the crystalline structure of pentacene active layer through atomic force microscope and X-ray diffraction, it was found that the adoption of water solvent in DNA solution, which played a key role in enhancing the field-effect mobility, was ascribed to both the elimination of the irreversible organic solvent-induced bulk-like phase transition of pentacene film and the diminution of a majority of charge trapping at interfaces in OFETs.

Behavior of pentacene initial nucleation on various dielectrics and its effect on carrier transport in organic field-effect transistor.

PubMed

Qi, Qiong; Yu, Aifang; Wang, Liangmin; Jiang, Chao

2010-11-01

The influence of dielectric surface energy on the initial nucleation and the growth of pentacene films as well as the electrical properties of the pentacene-based field-effect transistors are investigated. We have examined a range of organic and inorganic dielectrics with different surface energies, such as polycarbonate/SiO2, polystyrene/SiO2, and PMMA/SiO2 bi-layered dielectrics and also the bare SiO2 dielectric. Atomic force microscopy measurements of sub-monolayer and thick pentacene films indicated that the growth of pentacene film was in Stranski-Kranstanow growth mode on all the dielectrics. However, the initial nucleation density and the size of the first-layered pentacene islands deposited on different dielectrics are drastically influenced by the dielectric surface energy. With the increasing of the surface energy, the nucleation density increased and thus the average size of pentacene islands for the first mono-layer deposition decreased. The performance of fabricated pentacene-based thin film transistors was found to be highly related to nucleation density and the island size of deposited Pentacene film, and it had no relationship to the final particle size of the thick pentacene film. The field effect mobility of the thin film transistor could be achieved as high as 1.38 cm2Ns with on/off ratio over 3 x 10(7) on the PS/SiO2 where the lowest surface energy existed among all the dielectrics. For comparison, the values of mobility and on/off ratio were 0.42 cm2Ns and 1 x 10(6) for thin film transistor deposited directly on bare SiO2 having the highest surface energy.

Analysis of carrier transport and carrier trapping in organic diodes with polyimide-6,13-Bis(triisopropylsilylethynyl)pentacene double-layer by charge modulation spectroscopy and optical second harmonic generation measurement

NASA Astrophysics Data System (ADS)

Lim, Eunju; Taguchi, Dai; Iwamoto, Mitsumasa

2014-08-01

We studied the carrier transport and carrier trapping in indium tin oxide/polyimide (PI)/6,13-Bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene)/Au diodes by using charge modulation spectroscopy (CMS) and time-resolved electric field induced optical second harmonic generation (TR-EFISHG) measurements. TR-EFISHG directly probes the spatial carrier behaviors in the diodes, and CMS is useful in explaining the carrier motion with respect to energy. The results clearly indicate that the injected carriers move across TIPS-pentacene thorough the molecular energy states of TIPS-pentacene and accumulate at the PI/TIPS-pentacene interface. However, some carriers are trapped in the PI layers. These findings take into account the capacitance-voltage and current-voltage characteristics of the diodes.

Probing surface states in PbS nanocrystal films using pentacene field effect transistors: controlling carrier concentration and charge transport in pentacene.

PubMed

Park, Byoungnam; Whitham, Kevin; Bian, Kaifu; Lim, Yee-Fun; Hanrath, Tobias

2014-12-21

We used a bilayer field effect transistor (FET) consisting of a thin PbS nanocrystals (NCs) film interfaced with vacuum-deposited pentacene to probe trap states in NCs. We interpret the observed threshold voltage shift in context of charge carrier trapping by PbS NCs and relate the magnitude of the threshold voltage shift to the number of trapped carriers. We explored a series of NC surface ligands to modify the interface between PbS NCs and pentacene and demonstrate the impact of interface chemistry on charge carrier density and the FET mobility in a pentacene FET.

Study of carrier energetics in ITO/P(VDF-TrFE)/pentacene/Au diode by using electric-field-induced optical second harmonic generation measurement and charge modulation spectroscopy

NASA Astrophysics Data System (ADS)

Otsuka, Takako; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2017-02-01

By using electric-field-induced optical second harmonic generation (EFISHG) measurement and charge modulation spectroscopy (CMS), we studied carrier behavior and polarization reversal in ITO/ poly(vinylidene fluoride trifluoroethylene) (P(VDF-TrFE))/pentacene/Au diodes with a ferroelectric P(VDF-TrFE) layer in terms of carrier energetics. The current-voltage (I-V) characteristics of the diodes showed three-step polarization reversal in the dark. However, the I-V was totally different under illumination and exhibited two-step behavior. EFISHG probed the internal electric field in the pentacene layer and accounted for the polarization reversal change due to charge accumulation at the pentacene/P(VDF-TrFE) interface. CMS probed the related carrier energetics and indicated that exciton dissociation in pentacene molecular states governed carrier accumulation at the pentacene/ferroelectric interface, leading to different polarization reversal processes in the dark and under light illumination. Combining EFISHG measurement and CMS provides us a way to study carrier energetics that govern polarization reversal in ferroelectric P(VDF-TrFE)/pentacene diodes.

Exciton-dissociation and charge-recombination processes in pentacene/C60 solar cells: theoretical insight into the impact of interface geometry.

PubMed

Yi, Yuanping; Coropceanu, Veaceslav; Brédas, Jean-Luc

2009-11-04

The exciton-dissociation and charge-recombination processes in organic solar cells based on pentacene/C(60) heterojunctions are investigated by means of quantum-mechanical calculations. The electronic couplings and the rates of exciton dissociation and charge recombination have been evaluated for several geometrical configurations of the pentacene/C(60) complex, which are relevant to bilayer and bulk heterojunctions. The results suggest that, irrespective of the actual pentacene-fullerene orientation, both pentacene-based and C(60)-based excitons are able to dissociate efficiently. Also, in the case of parallel configurations of the molecules at the pentacene/C(60) interface, the decay of the lowest charge-transfer state to the ground state is calculated to be very fast; as a result, it can compete with the dissociation process into mobile charge carriers. Since parallel configurations are expected to be found more frequently in bulk heterojunctions than in bilayer heterojunctions, the performance of pentacene/C(60) bulk-heterojunction solar cells is likely to be more affected by charge recombination than that of bilayer devices.

Electron Transfer from Triplet State of TIPS-Pentacene Generated by Singlet Fission Processes to CH3NH3PbI3 Perovskite.

PubMed

Lee, Sangsu; Hwang, Daesub; Jung, Seok Il; Kim, Dongho

2017-02-16

To reveal the applicability of singlet fission processes in perovskite solar cell, we investigated electron transfer from TIPS-pentacene to CH 3 NH 3 PbI 3 (MAPbI 3 ) perovskite in film phase. Through the observation of the shorter fluorescence lifetime in TIPS-pentacene/MAPbI 3 perovskite bilayer film (5 ns) compared with pristine MAPbI 3 perovskite film (20 ns), we verified electron-transfer processes between TIPS-pentacene and MAPbI 3 perovskite. Furthermore, the observation of singlet fission processes, a faster decay rate, TIPS-pentacene cations, and the analysis of kinetic profiles of the intensity ratio between 500 and 525 nm in the TA spectra of the TIPS-pentacene/MAPbI 3 perovskite bilayer film indicate that electron transfer occurs from triplet state of TIPS-pentacene generated by singlet fission processes to MAPbI 3 perovskite conduction band. We believe that our results can provide useful information on the design of solar cells sensitized by singlet fission processes and pave the way for new types of perovskite solar cells.

High-Performance Simulations of the Diffusion Characteristics of a Pentacene Derivative on Gold Surfaces

NASA Astrophysics Data System (ADS)

Miller, Ryan; Larson, Amanda; Pohl, Karsten

Pentacene serves as a backbone for several molecules that provide attractive qualities for organic photovoltaic devices. One of these pentacene derivatives is 5 6,7-trithiapentacene-13-one (TTPO), which is unique in that it achieves its lowest energy configuration on Au(1 1 1) surfaces with the thiol group angled down towards the surface, allowing many molecules to pack closely together and form molecular nanowires. However, TTPO diffuses on flat surfaces, making it difficult for the self-assembly process to be initiated. With the help of the low-energy sites in surface defects and Au(7 8 8) step edges, TTPO molecules can be anchored in place on surfaces, allowing for chain formation to begin. By using high-performance Density Functional Theory based molecular dynamics calculations, the molecules can be shown to stay localized to these bonding sites and serve as a basis for chain formation. In addition, by simulating various temperatures with a Nose-Hoover thermostat, we can analyze how temperature affects anchoring ability and diffusion properties.

Two dimensional simulation of patternable conducting polymer electrode based organic thin film transistor

NASA Astrophysics Data System (ADS)

Nair, Shiny; Kathiresan, M.; Mukundan, T.

2018-02-01

Device characteristics of organic thin film transistor (OTFT) fabricated with conducting polyaniline:polystyrene sulphonic acid (PANi-PSS) electrodes, patterned by the Parylene lift-off method are systematically analyzed by way of two dimensional numerical simulation. The device simulation was performed taking into account field-dependent mobility, low mobility layer at the electrode-semiconductor interface, trap distribution in pentacene film and trapped charge at the organic/insulator interface. The electrical characteristics of bottom contact thin film transistor with PANi-PSS electrodes and pentacene active material is superior to those with palladium electrodes due to a lower charge injection barrier. Contact resistance was extracted in both cases by the transfer line method (TLM). The extracted charge concentration and potential profile from the two dimensional numerical simulation was used to explain the observed electrical characteristics. The simulated device characteristics not only matched the experimental electrical characteristics, but also gave an insight on the charge injection, transport and trap properties of the OTFTs as a function of different electrode materials from the perspectives of transistor operation.

Comment on ’Single Pentacene Molecules Detected by Fluorescence Excitation in a P-Terphenyl Crystal’

DTIC Science & Technology

1990-12-10

8217 NO 11 TITLE (include Security Classification) Comment on "Single Pentacene Molecules Detected by Fluorescence Excitation in a p-Terphenyl Crystal" 12...8217 {Continue on reverse it necessary and identify by block numboer) Using h--,Ihly efficient Fluorescence excitation spectroscov of individual pentacene ...molecular impurities in p-terphenvl crystals, we have observed that some pentacene defects exhibit spcntaneous spectral jumps in their resonance frequency at

Statistical Fine Structure in the Inhomogeneously Broadened Electronic Origin of Pentacene in p-Terphenyl.

DTIC Science & Technology

1988-01-29

Electronic Origin of Pentacene in p-Terphenyl by T. P. Carter, M. Manavi, and W. E. Moerner Prepared for Publication inDTIC Journal of Chemical Physics...Classification) Statistical Fine Structure in the Inhomogeneously Broadened Electronic Origin of Pentacene in p-Terphenyl 12. PERSONAL AUTHOR(S) T. P...of pentacene in p-terphenyl using laser FM spectroscopy. Statistical fine structure is time-independent structure on the inhomogeneous line caused by

Pulsed electron nuclear double resonance studies of the photoexcited triplet state of pentacene in p-terphenyl crystals at room temperature.

PubMed

Yago, Tomoaki; Link, Gerhard; Kothe, Gerd; Lin, Tien-Sung

2007-09-21

Pulsed electron nuclear double resonance (ENDOR) using a modified Davies-type [Phys. Lett. 47A, 1 (1974)] sequence is employed to study the hyperfine (HF) structure of the photoexcited triplet state of pentacene dispersed in protonated and deuterated p-terphenyl single crystals. The strong electron spin polarization and long phase memory time of triplet pentacene enable us to perform the ENDOR measurements on the S=1 spin system at room temperature. Proton HF tensor elements and spin density values of triplet pentacene are extracted from a detailed angular-dependent study in which the orientation of the magnetic field is varied systematically in two different pentacene planes. Analysis reveals that the pentacene molecule is no longer planar in the p-terphenyl host lattice. The distortion is more pronounced in the deuterated crystal where the unit cell dimensions are slightly smaller than those of the protonated crystal.

Fast and inexpensive synthesis of pentacene with high yield using 6,13-pentacenequinone as precursor

NASA Astrophysics Data System (ADS)

Mota, María L.; Rodriguez, Bibiana; Carrillo, Amanda; Ambrosio, Roberto C.; Luque, Priscy A.; Mireles, Marcela; Vivaldo, Israel; Quevedo, Manuel A.

2018-02-01

Pentacene is an important semiconductor in the field of organic electronics. In this work is presented an alternative synthesis procedure to obtain pentacene from 6,13-pentacenequinone as a precursor. Synthesis of pentacene was performed in two reactions, Diels-Adler cycloaddition of 6,13-pentacenequinone followed by 6,13-pentacenequinone reduction to pentacene, employing LiAlH4 as reducing agent. The products were characterized by Fourier Transform Infrared Spectroscopy (FTIR), 1H-Nuclear Magnetic Resonance Spectroscopy (1H-NMR), X-Ray Diffraction (XRD), Thermogravimetric Analysis (TGA) and Ultraviolet-Visible Spectroscopy (UV-VIS). In this work, 6,13-pentacenequinone was synthetized with a high yield (55%) using an alternative method. The optimization process resulted in an overall reduction of reaction time while exhibiting high yield. The method presented here provides an affordable pentacene synthesis route with high purity, which can be further applied for research and development of organic electronic applications.

The effect of thermal annealing on pentacene thin film transistor with micro contact printing.

PubMed

Shin, Hong-Sik; Yun, Ho-Jin; Baek, Kyu-Ha; Ham, Yong-Hyun; Park, Kun-Sik; Kim, Dong-Pyo; Lee, Ga-Won; Lee, Hi-Deok; Lee, Kijun; Do, Lee-Mi

2012-07-01

We used micro contact printing (micro-CP) to fabricate inverted coplanar pentacene thin film transistors (TFTs) with 1-microm channels. The patterning of micro-scale source/drain electrodes without etch process was successfully achieved using Polydimethylsiloxane (PDMS) elastomer stamp. We used the Ag nano particle ink as an electrode material, and the sheet resistance and surface roughness of the Ag electrodes were effectively reduced with the 2-step thermal annealing on a hotplate, which improved the mobility, the on-off ratio, and the subthreshold slope (SS) of the pentacene TFTs. In addition, the device annealing on a hotplate in a N2 atmosphere for 30 sec can enhance the off-current and the mobility properties of OTFTs without damaging the pentacene thin films and increase the adhesion between pentacene and dielectric layer (SiO2), which was investigated with the pentacene films phase change of the XRD spectrum after device annealing.

Distinct properties of the triplet pair state from singlet fission

DOE PAGES

Trinh, M. Tuan; Pinkard, Andrew; Pun, Andrew B.; ...

2017-07-14

Singlet fission, the conversion of a singlet exciton (S 1) to two triplets (2 × T 1), may increase the solar energy conversion efficiency beyond the Shockley-Queisser limit. This process is believed to involve the correlated triplet pair state 1(TT). Despite extensive research, the nature of the 1(TT) state and its spectroscopic signature remain actively debated. We use an end-connected pentacene dimer (BP0) as a model system and show evidence for a tightly bound 1(TT) state. It is characterized in the near-infrared (IR) region (~1.0 eV) by a distinct excited-state absorption (ESA) spectral feature, which closely resembles that of themore » S 1 state; both show vibronic progressions of the aromatic ring breathing mode. We assign these near-IR spectra to 1(TT)→S n and S 1→S n' transitions; S n and S n' likely come from the antisymmetric and symmetric linear combinations, respectively, of the S 2 state localized on each pentacene unit in the dimer molecule. The 1(TT)→S n transition is an indicator of the intertriplet electronic coupling strength, because inserting a phenylene spacer or twisting the dihedral angle between the two pentacene chromophores decreases the intertriplet electronic coupling and diminishes this ESA peak. In addition to spectroscopic signature, the tightly bound 1(TT) state also shows chemical reactivity that is distinctively different from that of an individual T 1 state. Using an electron-accepting iron oxide molecular cluster [Fe 8O 4] linked to the pentacene or pentacene dimer (BP0), we show that electron transfer to the cluster occurs efficiently from an individual T 1 in pentacene but not from the tightly bound 1(TT) state. Thus, reducing intertriplet electronic coupling in 1(TT) via molecular design might be necessary for the efficient harvesting of triplets from intramolecular singlet fission.« less

Distinct properties of the triplet pair state from singlet fission.

PubMed

Trinh, M Tuan; Pinkard, Andrew; Pun, Andrew B; Sanders, Samuel N; Kumarasamy, Elango; Sfeir, Matthew Y; Campos, Luis M; Roy, Xavier; Zhu, X-Y

2017-07-01

Singlet fission, the conversion of a singlet exciton (S 1 ) to two triplets (2 × T 1 ), may increase the solar energy conversion efficiency beyond the Shockley-Queisser limit. This process is believed to involve the correlated triplet pair state 1 (TT). Despite extensive research, the nature of the 1 (TT) state and its spectroscopic signature remain actively debated. We use an end-connected pentacene dimer (BP0) as a model system and show evidence for a tightly bound 1 (TT) state. It is characterized in the near-infrared (IR) region (~1.0 eV) by a distinct excited-state absorption (ESA) spectral feature, which closely resembles that of the S 1 state; both show vibronic progressions of the aromatic ring breathing mode. We assign these near-IR spectra to 1 (TT)→S n and S 1 →S n' transitions; S n and S n' likely come from the antisymmetric and symmetric linear combinations, respectively, of the S 2 state localized on each pentacene unit in the dimer molecule. The 1 (TT)→S n transition is an indicator of the intertriplet electronic coupling strength, because inserting a phenylene spacer or twisting the dihedral angle between the two pentacene chromophores decreases the intertriplet electronic coupling and diminishes this ESA peak. In addition to spectroscopic signature, the tightly bound 1 (TT) state also shows chemical reactivity that is distinctively different from that of an individual T 1 state. Using an electron-accepting iron oxide molecular cluster [Fe 8 O 4 ] linked to the pentacene or pentacene dimer (BP0), we show that electron transfer to the cluster occurs efficiently from an individual T 1 in pentacene but not from the tightly bound 1 (TT) state. Thus, reducing intertriplet electronic coupling in 1 (TT) via molecular design might be necessary for the efficient harvesting of triplets from intramolecular singlet fission.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Trinh, M. Tuan; Pinkard, Andrew; Pun, Andrew B.

Singlet fission, the conversion of a singlet exciton (S 1) to two triplets (2 × T 1), may increase the solar energy conversion efficiency beyond the Shockley-Queisser limit. This process is believed to involve the correlated triplet pair state 1(TT). Despite extensive research, the nature of the 1(TT) state and its spectroscopic signature remain actively debated. We use an end-connected pentacene dimer (BP0) as a model system and show evidence for a tightly bound 1(TT) state. It is characterized in the near-infrared (IR) region (~1.0 eV) by a distinct excited-state absorption (ESA) spectral feature, which closely resembles that of themore » S 1 state; both show vibronic progressions of the aromatic ring breathing mode. We assign these near-IR spectra to 1(TT)→S n and S 1→S n' transitions; S n and S n' likely come from the antisymmetric and symmetric linear combinations, respectively, of the S 2 state localized on each pentacene unit in the dimer molecule. The 1(TT)→S n transition is an indicator of the intertriplet electronic coupling strength, because inserting a phenylene spacer or twisting the dihedral angle between the two pentacene chromophores decreases the intertriplet electronic coupling and diminishes this ESA peak. In addition to spectroscopic signature, the tightly bound 1(TT) state also shows chemical reactivity that is distinctively different from that of an individual T 1 state. Using an electron-accepting iron oxide molecular cluster [Fe 8O 4] linked to the pentacene or pentacene dimer (BP0), we show that electron transfer to the cluster occurs efficiently from an individual T 1 in pentacene but not from the tightly bound 1(TT) state. Thus, reducing intertriplet electronic coupling in 1(TT) via molecular design might be necessary for the efficient harvesting of triplets from intramolecular singlet fission.« less

Distinct properties of the triplet pair state from singlet fission

PubMed Central

Trinh, M. Tuan; Pinkard, Andrew; Pun, Andrew B.; Sanders, Samuel N.; Kumarasamy, Elango; Sfeir, Matthew Y.; Campos, Luis M.; Roy, Xavier; Zhu, X.-Y.

2017-01-01

Singlet fission, the conversion of a singlet exciton (S1) to two triplets (2 × T1), may increase the solar energy conversion efficiency beyond the Shockley-Queisser limit. This process is believed to involve the correlated triplet pair state 1(TT). Despite extensive research, the nature of the 1(TT) state and its spectroscopic signature remain actively debated. We use an end-connected pentacene dimer (BP0) as a model system and show evidence for a tightly bound 1(TT) state. It is characterized in the near-infrared (IR) region (~1.0 eV) by a distinct excited-state absorption (ESA) spectral feature, which closely resembles that of the S1 state; both show vibronic progressions of the aromatic ring breathing mode. We assign these near-IR spectra to 1(TT)→Sn and S1→Sn′ transitions; Sn and Sn′ likely come from the antisymmetric and symmetric linear combinations, respectively, of the S2 state localized on each pentacene unit in the dimer molecule. The 1(TT)→Sn transition is an indicator of the intertriplet electronic coupling strength, because inserting a phenylene spacer or twisting the dihedral angle between the two pentacene chromophores decreases the intertriplet electronic coupling and diminishes this ESA peak. In addition to spectroscopic signature, the tightly bound 1(TT) state also shows chemical reactivity that is distinctively different from that of an individual T1 state. Using an electron-accepting iron oxide molecular cluster [Fe8O4] linked to the pentacene or pentacene dimer (BP0), we show that electron transfer to the cluster occurs efficiently from an individual T1 in pentacene but not from the tightly bound 1(TT) state. Thus, reducing intertriplet electronic coupling in 1(TT) via molecular design might be necessary for the efficient harvesting of triplets from intramolecular singlet fission. PMID:28740866

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lim, Eunju, E-mail: elim@dankook.ac.kr, E-mail: taguchi.d.aa@m.titech.ac.jp, E-mail: iwamoto@pe.titech.ac.jp; Taguchi, Dai, E-mail: elim@dankook.ac.kr, E-mail: taguchi.d.aa@m.titech.ac.jp, E-mail: iwamoto@pe.titech.ac.jp; Iwamoto, Mitsumasa, E-mail: elim@dankook.ac.kr, E-mail: taguchi.d.aa@m.titech.ac.jp, E-mail: iwamoto@pe.titech.ac.jp

We studied the carrier transport and carrier trapping in indium tin oxide/polyimide (PI)/6,13-Bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene)/Au diodes by using charge modulation spectroscopy (CMS) and time-resolved electric field induced optical second harmonic generation (TR-EFISHG) measurements. TR-EFISHG directly probes the spatial carrier behaviors in the diodes, and CMS is useful in explaining the carrier motion with respect to energy. The results clearly indicate that the injected carriers move across TIPS-pentacene thorough the molecular energy states of TIPS-pentacene and accumulate at the PI/TIPS-pentacene interface. However, some carriers are trapped in the PI layers. These findings take into account the capacitance-voltage and current-voltage characteristics of themore » diodes.« less

Performance enhancement of pentacene-based organic thin-film transistors using 6,13-pentacenequinone as a carrier injection interlayer

NASA Astrophysics Data System (ADS)

Fan, Ching-Lin; Lin, Wei-Chun; Chen, Hao-Wei

2018-06-01

This work demonstrates pentacene-based organic thin-film transistors (OTFTs) fabricated by inserting a 6,13-pentacenequinone (PQ) carrier injection layer between the source/drain (S/D) metal Au electrodes and pentacene channel layer. Compared to devices without a PQ layer, the performance characteristics including field-effect mobility, threshold voltage, and On/Off current ratio were significantly improved for the device with a 5-nm-thick PQ interlayer. These improvements are attributed to significant reduction of hole barrier height at the Au/pentacene channel interfaces. Therefore, it is believed that using PQ as the carrier injection layer is a good candidate to improve the pentacene-based OTFTs electrical performance.

High Performance Crystalline Organic Transistors and Circuit

DTIC Science & Technology

2009-10-14

this material into pentacene -based OFETs, low voltage operation is possible. 3 Figure 1: Device structure for a low voltage pentacene OFET...issues with the first SiO Z OPentacene Au Pentacene ZrO2 AuPd SiO2 4 film. Bilayer dielectrics exhibit lower defect-related leakage...effects, as pinholes or other defects in one layer may be isolated by the other layer. 350 Å of pentacene was thermally evaporated on the ZrO2 dielectric

X-Ray Irradiation Effects in Top Contact, Pentacene Based Field Effect Transistors for Space Related Applications

DTIC Science & Technology

2006-01-01

Journal Article POSTPRINT 3. DATES COVERED (From - To) 2006 4. TITLE AND SUBTITLE X-ray irradiation effects in top contact, pentacene based field 5a...Preliminary studies of the effect of x-ray irradiation, typically used to simulate radiation effects in space, on top contract, pentacene based field effect...irradiation, radiation, radiation effects, pentacene 16. SECURITY CLASSIFICATION OF: 17. LIMITATION OF ABSTRACT 18. NUMBER OF PAGES 19a. NAME OF

Pentacene Derivatives as Red Emitters in Organic Light Emitting Devices.

DTIC Science & Technology

1999-12-16

20000223 076 1 2 3 4 5 6 12 13 Docket No.:N.C. 79 914 ^-^ V^ U (J Inventor’s Name: Us, Cnsafuln Picolo, ffideyuki Murata, Zakya H.™" ^^^ PENTACENE ...materials doped 10 with pentacene derivatives. 11 2. Description of the Related Art Organic electroluminescent devices have been the subject of...wavelengths. Summary of the Invention It has now been discovered that pentacene derivatives exhibit very narrow emission spectra and produce a very pure

Effects of (NH4)2S x treatment on the surface properties of SiO2 as a gate dielectric for pentacene thin-film transistor applications

NASA Astrophysics Data System (ADS)

Hung, Cheng-Chun; Lin, Yow-Jon

2018-01-01

The effect of (NH4)2S x treatment on the surface properties of SiO2 is studied. (NH4)2S x treatment leads to the formation of S-Si bonds on the SiO2 surface that serves to reduce the number of donor-like trap states, inducing the shift of the Fermi level toward the conduction band minimum. A finding in this case is the noticeably reduced value of the SiO2 capacitance as the sulfurated layer is formed at the SiO2 surface. The effect of SiO2 layers with (NH4)2S x treatment on the carrier transport behaviors for the pentacene/SiO2-based organic thin-film transistor (OTFT) is also studied. The pentacene/as-cleaned SiO2-based OTFT shows depletion-mode behavior, whereas the pentacene/(NH4)2S x -treated SiO2-based OTFT exhibits enhancement-mode behavior. Experimental identification confirms that the depletion-/enhancement-mode conversion is due to the dominance competition between donor-like trap states in SiO2 near the pentacene/SiO2 interface and acceptor-like trap states in the pentacene channel. A sulfurated layer between pentacene and SiO2 is expected to give significant contributions to carrier transport for pentacene/SiO2-based OTFTs.

pn-Heterojunction effects of perylene tetracarboxylic diimide derivatives on pentacene field-effect transistor.

PubMed

Yu, Seong Hun; Kang, Boseok; An, Gukil; Kim, BongSoo; Lee, Moo Hyung; Kang, Moon Sung; Kim, Hyunjung; Lee, Jung Heon; Lee, Shichoon; Cho, Kilwon; Lee, Jun Young; Cho, Jeong Ho

2015-01-28

We investigated the heterojunction effects of perylene tetracarboxylic diimide (PTCDI) derivatives on the pentacene-based field-effect transistors (FETs). Three PTCDI derivatives with different substituents were deposited onto pentacene layers and served as charge transfer dopants. The deposited PTCDI layer, which had a nominal thickness of a few layers, formed discontinuous patches on the pentacene layers and dramatically enhanced the hole mobility in the pentacene FET. Among the three PTCDI molecules tested, the octyl-substituted PTCDI, PTCDI-C8, provided the most efficient hole-doping characteristics (p-type) relative to the fluorophenyl-substituted PTCDIs, 4-FPEPTC and 2,4-FPEPTC. The organic heterojunction and doping characteristics were systematically investigated using atomic force microscopy, 2D grazing incidence X-ray diffraction studies, and ultraviolet photoelectron spectroscopy. PTCDI-C8, bearing octyl substituents, grew laterally on the pentacene layer (2D growth), whereas 2,4-FPEPTC, with fluorophenyl substituents, underwent 3D growth. The different growth modes resulted in different contact areas and relative orientations between the pentacene and PTCDI molecules, which significantly affected the doping efficiency of the deposited adlayer. The differences between the growth modes and the thin-film microstructures in the different PTCDI patches were attributed to a mismatch between the surface energies of the patches and the underlying pentacene layer. The film-morphology-dependent doping effects observed here offer practical guidelines for achieving more effective charge transfer doping in thin-film transistors.

Experimental and numerical investigation of contact-area-limited doping for top-contact pentacene thin-film transistors with Schottky contact.

PubMed

Noda, Kei; Wada, Yasuo; Toyabe, Toru

2015-10-28

Effects of contact-area-limited doping for pentacene thin-film transistors with a bottom-gate, top-contact configuration were investigated. The increase in the drain current and the effective field-effect mobility was achieved by preparing hole-doped layers underneath the gold contact electrodes by coevaporation of pentacene and 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ), confirmed by using a thin-film organic transistor advanced simulator (TOTAS) incorporating Schottky contact with a thermionic field emission (TFE) model. Although the simulated electrical characteristics fit the experimental results well only in the linear regime of the transistor operation, the barrier height for hole injection and the gate-voltage-dependent hole mobility in the pentacene transistors were evaluated with the aid of the device simulation. This experimental data analysis with the simulation indicates that the highly-doped semiconducting layers prepared in the contact regions can enhance the charge carrier injection into the active semiconductor layer and concurrent trap filling in the transistor channel, caused by the mitigation of a Schottky energy barrier. This study suggests that both the contact-area-limited doping and the device simulation dealing with Schottky contact are indispensable in designing and developing high-performance organic thin-film transistors.

The role of the van der Waals interactions in the adsorption of anthracene and pentacene on the Ag(111) surface

NASA Astrophysics Data System (ADS)

Morbec, Juliana M.; Kratzer, Peter

2017-01-01

Using first-principles calculations based on density-functional theory (DFT), we investigated the effects of the van der Waals (vdW) interactions on the structural and electronic properties of anthracene and pentacene adsorbed on the Ag(111) surface. We found that the inclusion of vdW corrections strongly affects the binding of both anthracene/Ag(111) and pentacene/Ag(111), yielding adsorption heights and energies more consistent with the experimental results than standard DFT calculations with generalized gradient approximation (GGA). For anthracene/Ag(111) the effect of the vdW interactions is even more dramatic: we found that "pure" DFT-GGA calculations (without including vdW corrections) result in preference for a tilted configuration, in contrast to the experimental observations of flat-lying adsorption; including vdW corrections, on the other hand, alters the binding geometry of anthracene/Ag(111), favoring the flat configuration. The electronic structure obtained using a self-consistent vdW scheme was found to be nearly indistinguishable from the conventional DFT electronic structure once the correct vdW geometry is employed for these physisorbed systems. Moreover, we show that a vdW correction scheme based on a hybrid functional DFT calculation (HSE) results in an improved description of the highest occupied molecular level of the adsorbed molecules.

Self-Limited Growth in Pentacene Thin Films

PubMed Central

2017-01-01

Pentacene is one of the most studied organic semiconducting materials. While many aspects of the film formation have already been identified in very thin films, this study provides new insight into the transition from the metastable thin-film phase to bulk phase polymorphs. This study focuses on the growth behavior of pentacene within thin films as a function of film thickness ranging from 20 to 300 nm. By employing various X-ray diffraction methods, combined with supporting atomic force microscopy investigations, one crystalline orientation for the thin-film phase is observed, while three differently tilted bulk phase orientations are found. First, bulk phase crystallites grow with their 00L planes parallel to the substrate surface; second, however, crystallites tilted by 0.75° with respect to the substrate are found, which clearly dominate the former in ratio; third, a different bulk phase polymorph with crystallites tilted by 21° is found. The transition from the thin-film phase to the bulk phase is rationalized by the nucleation of the latter at crystal facets of the thin-film-phase crystallites. This leads to a self-limiting growth of the thin-film phase and explains the thickness-dependent phase behavior observed in pentacene thin films, showing that a large amount of material is present in the bulk phase much earlier during the film growth than previously thought. PMID:28287698

Self-Limited Growth in Pentacene Thin Films.

PubMed

Pachmajer, Stefan; Jones, Andrew O F; Truger, Magdalena; Röthel, Christian; Salzmann, Ingo; Werzer, Oliver; Resel, Roland

2017-04-05

Pentacene is one of the most studied organic semiconducting materials. While many aspects of the film formation have already been identified in very thin films, this study provides new insight into the transition from the metastable thin-film phase to bulk phase polymorphs. This study focuses on the growth behavior of pentacene within thin films as a function of film thickness ranging from 20 to 300 nm. By employing various X-ray diffraction methods, combined with supporting atomic force microscopy investigations, one crystalline orientation for the thin-film phase is observed, while three differently tilted bulk phase orientations are found. First, bulk phase crystallites grow with their 00L planes parallel to the substrate surface; second, however, crystallites tilted by 0.75° with respect to the substrate are found, which clearly dominate the former in ratio; third, a different bulk phase polymorph with crystallites tilted by 21° is found. The transition from the thin-film phase to the bulk phase is rationalized by the nucleation of the latter at crystal facets of the thin-film-phase crystallites. This leads to a self-limiting growth of the thin-film phase and explains the thickness-dependent phase behavior observed in pentacene thin films, showing that a large amount of material is present in the bulk phase much earlier during the film growth than previously thought.

Surface-directed molecular assembly of pentacene on monolayer graphene for high-performance organic transistors.

PubMed

Lee, Wi Hyoung; Park, Jaesung; Sim, Sung Hyun; Lim, Soojin; Kim, Kwang S; Hong, Byung Hee; Cho, Kilwon

2011-03-30

Organic electronic devices that use graphene electrodes have received considerable attention because graphene is regarded as an ideal candidate electrode material. Transfer and lithographic processes during fabrication of patterned graphene electrodes typically leave polymer residues on the graphene surfaces. However, the impact of these residues on the organic semiconductor growth mechanism on graphene surface has not been reported yet. Here, we demonstrate that polymer residues remaining on graphene surfaces induce a stand-up orientation of pentacene, thereby controlling pentacene growth such that the molecular assembly is optimal for charge transport. Thus, pentacene field-effect transistors (FETs) using source/drain monolayer graphene electrodes with polymer residues show a high field-effect mobility of 1.2 cm(2)/V s. In contrast, epitaxial growth of pentacene having molecular assembly of lying-down structure is facilitated by π-π interaction between pentacene and the clean graphene electrode without polymer residues, which adversely affects lateral charge transport at the interface between electrode and channel. Our studies provide that the obtained high field-effect mobility in pentacene FETs using monolayer graphene electrodes arises from the extrinsic effects of polymer residues as well as the intrinsic characteristics of the highly conductive, ultrathin two-dimensional monolayer graphene electrodes.

Structural features of the adsorption layer of pentacene on the graphite surface and the PMMA/graphite hybrid surface

NASA Astrophysics Data System (ADS)

Fadeeva, A. I.; Gorbunov, V. A.; Litunenko, T. A.

2017-08-01

Using the molecular dynamics and the Monte Carlo methods, we have studied the structural features and growth mechanism of the pentacene film on graphite and polymethylmethacrylate /graphite surfaces. Monolayer capacity and molecular area, optimal angles between the pentacene molecules and graphite and PMMA/graphite surfaces as well as the characteristic angles between the neighboring pentacene molecules in the adsorption layer were estimated. It is shown that the orientation of the pentacene molecules in the film is determined by a number of factors, including the surface concentration of the molecules, relief of the surface, presence or absence of the polymer layer and its thickness. The pentacene molecules adsorbed on the graphite surface keep a horizontal position relative to the long axis at any surface coverage/thickness of the film. In the presence of the PMMA layer on the graphite, the increase of the number of pentacene molecules as well as the thickness of the PMMA layer induce the change of molecular orientation from predominantly horizontal to vertical one. The reason for such behavior is supposed to be the roughness of the PMMA surface.

Detection and Spectroscopy of Single Pentacene Molecules in a p- Terphenyl Crystal by Means of Fluorescence Excitation

DTIC Science & Technology

1991-07-22

suggesting that the effect may be ite td’ phonon-assisted transitions of local degrees of freedom around the pentacene defect whose source remains to...the effect may be due to phonon-assisted transitions of local degrees of freedom around the pentacene defect whose source remains to be identified...single molecule of pentacene in p-terphenyl is an exquisitely sensitive probe of the detailed local environment around the impurity molecule. It appears

High Performance Crystalline Organic Transistors and Circuit

DTIC Science & Technology

2011-08-02

pentacene -based OFETs, low voltage operation is possible. 3 Figure 1: Device structure for a low voltage pentacene OFET using a ZrO2 gate...first SiO Z OPentacene Au Pentacene ZrO2 AuPd SiO2 4 film. Bilayer dielectrics exhibit lower defect-related leakage effects, as pinholes or...other defects in one layer may be isolated by the other layer. 350 Å of pentacene was thermally evaporated on the ZrO2 dielectric at a rate of 0.1 Å

High mobility organic field-effect transistor based on water-soluble deoxyribonucleic acid via spray coating

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shi, Wei; Han, Shijiao; Huang, Wei

High mobility organic field-effect transistors (OFETs) by inserting water-soluble deoxyribonucleic acid (DNA) buffer layer between electrodes and pentacene film through spray coating process were fabricated. Compared with the OFETs incorporated with DNA in the conventional organic solvents of ethanol and methanol: water mixture, the water-soluble DNA based OFET exhibited an over four folds enhancement of field-effect mobility from 0.035 to 0.153 cm{sup 2}/Vs. By characterizing the surface morphology and the crystalline structure of pentacene active layer through atomic force microscope and X-ray diffraction, it was found that the adoption of water solvent in DNA solution, which played a key role inmore » enhancing the field-effect mobility, was ascribed to both the elimination of the irreversible organic solvent-induced bulk-like phase transition of pentacene film and the diminution of a majority of charge trapping at interfaces in OFETs.« less

Pentacene Schottky diodes studied by impedance spectroscopy: Doping properties and trap response

NASA Astrophysics Data System (ADS)

Pahner, Paul; Kleemann, Hans; Burtone, Lorenzo; Tietze, Max L.; Fischer, Janine; Leo, Karl; Lüssem, Björn

2013-11-01

We study doping properties and charge carrier trap distributions in pentacene Schottky diodes doped by the fluorinated fullerene derivate C60F36 and 2,2'-(perdiylidene)dimalononitrile (F6-TCNNQ) upon small signal excitation. We show that the charge carrier depletion zones present in these Schottky diodes are tunable by the applied bias and temperature. Mott-Schottky evaluations yield reduced doping efficiencies and dopant activation energies between 19 and 54 meV. In the low-frequency regime, we resolve additional capacitive contributions from inherent charge carrier traps. A Gaussian distributed trap center 0.6 eV above the hole transport level with a density in the range of 1016 cm-3 depending on the material purity is found to be an intrinsic feature of the pentacene matrix. Upon doping, the deep Gaussian trap center saturates in density and broad exponentially tailing trap distributions arise. Subsequent ultraviolet photoelectron spectroscopy measurements are conducted to inspect for energetic broadening due to doping.

Transport characteristics in Au/pentacene/Au diodes

NASA Astrophysics Data System (ADS)

Hayashi, Toshiaki; Naka, Akiyoshi; Hiroki, Masanobu; Yokota, Tomoyuki; Someya, Takao; Fujiwara, Akira

2018-03-01

We have used scanning and transmission electron microscopes (SEM and TEM) to study the structure of a pentacene thin film grown on a Au layer with and shown that it consists of randomly oriented amorphous pentacene clusters. We have also investigated the transport properties of amorphous pentacene in a metal-semiconductor-metal (MSM) diode structure and shown that the current is logarithmically proportional to the square root of the applied voltage, which indicates that transport occurs as the result of hopping between localized sites randomly distributed in space and energy.

Stabilizing Pentacene By Cyclopentannulation.

PubMed

Bheemireddy, Sambasiva R; Ubaldo, Pamela C; Rose, Peter W; Finke, Aaron D; Zhuang, Junpeng; Wang, Lichang; Plunkett, Kyle N

2015-12-21

A new class of stabilized pentacene derivatives with externally fused five-membered rings are prepared by means of a key palladium-catalyzed cyclopentannulation step. The target compounds are synthesized by chemical manipulation of a partially saturated 6,13-dibromopentacene precursor that can be fully aromatized in a final step through a DDQ-mediated dehydrogenation reaction (DDQ=2,3-dichloro-5,6-dicyano-1,4-benzoquinone). The new 1,2,8,9-tetraaryldicyclopenta[fg,qr]pentacene derivatives have narrow energy gaps of circa 1.2 eV and behave as strong electron acceptors with lowest unoccupied molecular orbital energies between -3.81 and -3.90 eV. Photodegradation studies reveal the new compounds are more photostable than 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene). © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Graphene/Pentacene Barristor with Ion-Gel Gate Dielectric: Flexible Ambipolar Transistor with High Mobility and On/Off Ratio.

PubMed

Oh, Gwangtaek; Kim, Jin-Soo; Jeon, Ji Hoon; Won, EunA; Son, Jong Wan; Lee, Duk Hyun; Kim, Cheol Kyeom; Jang, Jingon; Lee, Takhee; Park, Bae Ho

2015-07-28

High-quality channel layer is required for next-generation flexible electronic devices. Graphene is a good candidate due to its high carrier mobility and unique ambipolar transport characteristics but typically shows a low on/off ratio caused by gapless band structure. Popularly investigated organic semiconductors, such as pentacene, suffer from poor carrier mobility. Here, we propose a graphene/pentacene channel layer with high-k ion-gel gate dielectric. The graphene/pentacene device shows both high on/off ratio and carrier mobility as well as excellent mechanical flexibility. Most importantly, it reveals ambipolar behaviors and related negative differential resistance, which are controlled by external bias. Therefore, our graphene/pentacene barristor with ion-gel gate dielectric can offer various flexible device applications with high performances.

Morphology and current-voltage characteristics of nanostructured pentacene thin films probed by atomic force microscopy.

PubMed

Zorba, S; Le, Q T; Watkins, N J; Yan, L; Gao, Y

2001-09-01

Atomic force microscopy was used to study the growth modes (on SiO2, MoS2, and Au substrates) and the current-voltage (I-V) characteristics of organic semiconductor pentacene. Pentacene films grow on SiO2 substrate in a layer-by-layer manner with full coverage at an average thickness of 20 A and have the highest degree of molecular ordering with large dendritic grains among the pentacene films deposited on the three different substrates. Films grown on MoS2 substrate reveal two different growth modes, snowflake-like growth and granular growth, both of which seem to compete with each other. On the other hand, films deposited on Au substrate show granular structure for thinner coverages (no crystal structure) and dendritic growth for higher coverages (crystal structure). I-V measurements were performed with a platinum tip on a pentacene film deposited on a Au substrate. The I-V curves on pentacene film reveal symmetric tunneling type character. The field dependence of the current indicates that the main transport mechanism at high field intensities is hopping (Poole-Frenkel effect). From these measurements, we have estimated a field lowering coefficient of 9.77 x 10(-6) V-1/2 m1/2 and an ideality factor of 18 for pentacene.

Formation of intra-island grain boundaries in pentacene monolayers.

PubMed

Zhang, Jian; Wu, Yu; Duhm, Steffen; Rabe, Jürgen P; Rudolf, Petra; Koch, Norbert

2011-12-21

To assess the formation of intra-island grain boundaries during the early stages of pentacene film growth, we studied sub-monolayers of pentacene on pristine silicon oxide and silicon oxide with high pinning centre density (induced by UV/O(3) treatment). We investigated the influence of the kinetic energy of the impinging molecules on the sub-monolayer growth by comparing organic molecular beam deposition (OMBD) and supersonic molecular beam deposition (SuMBD). For pentacene films fabricated by OMBD, higher pentacene island-density and higher polycrystalline island density were observed on UV/O(3)-treated silicon oxide as compared to pristine silicon oxide. Pentacene films deposited by SuMBD exhibited about one order of magnitude lower island- and polycrystalline island densities compared to OMBD, on both types of substrates. Our results suggest that polycrystalline growth of single islands on amorphous silicon oxide is facilitated by structural/chemical surface pinning centres, which act as nucleation centres for multiple grain formation in a single island. Furthermore, the overall lower intra-island grain boundary density in pentacene films fabricated by SuMBD reduces the number of charge carrier trapping sites specific to grain boundaries and should thus help achieving higher charge carrier mobilities, which are advantageous for their use in organic thin-film transistors.

Graphene-based electrodes for enhanced organic thin film transistors based on pentacene.

PubMed

Basu, Sarbani; Lee, Mu Chen; Wang, Yeong-Her

2014-08-21

This paper presents 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene) and pentacene-based organic thin film transistors (OTFTs) with monolayer graphene source-drain (S-D) electrodes. The electrodes are patterned using conventional photolithographic techniques combined with reactive ion etching. The monolayer graphene film grown by chemical vapor deposition on Cu foil was transferred on a Si dioxide surface using a polymer-supported transfer method to fabricate bottom-gate, bottom-contact OTFTs. The pentacene OTFTs with graphene S-D contacts exhibited superior performance with a mobility of 0.1 cm(2) V(-1) s(-1) and an on-off ratio of 10(5) compared with OTFTs with Au-based S-D contacts, which had a mobility of 0.01 cm(2) V(-1) s(-1) and an on-off ratio of 10(3). The crystallinity, grain size, and microscopic defects (or the number of layers of graphene films) of the TIPS-pentacene/pentacene films were analyzed by X-ray diffraction spectroscopy, atomic force microscopy, and Raman spectroscopy, respectively. The feasibility of using graphene as an S-D electrode in OTFTs provides an alternative material with high carrier injection efficiency, chemical stability, and excellent interface properties with organic semiconductors, thus exhibiting improved device performance of C-based electronic OTFTs at a reduced cost.

Tips pentacene crystal alignment for improving performance of solution processed organic thin film transistors

NASA Astrophysics Data System (ADS)

He, Zhengran

A newly-developed p-type organic semiconductor 6,13-bis (triisopropylsilylethynyl) pentacene (TIPS pentacene) demonstrates various advantages such as high mobility, air stability and solution processibility, but at the same time its application is restricted by major issues, such as crystal misorientation and performance variation of organic thin-film transistors (OTFTs). This dissertation demonstrates several different approaches to address these issues. As a result, both crystal orientation and areal coverage can be effectively improved, leading to an enhancement of average mobility and performance consistency of OTFTs. Chapter 1 presents an introduction and background of this dissertation. Chapter 2 explores the usage of inorganic silica nanoparticles to manipulate the morphology of TIPS pentacene thin films and the performance of solution-processed organic OTFTs. The resultant drop-cast films yield improved morphological uniformity at ~10% SiO2 loading, which also leads to a 3-fold increase in average mobility and nearly 4-times reduction in the ratio of standard deviation of mobility (μStdev) to average mobility (μAvg). The experimental results suggest that the SiO2 nanoparticles mostly aggregate at TIPS pentacene grain boundaries, and that 10% nanoparticle concentration effectively reduces the undesirable crystal misorientation without considerably compromising TIPS pentacene crystallinity. Chapter 3 discusses the utilization of air flow to effectively reduce the TIPS pentacene crystal anisotropy and enhance performance consistency in OTFTs. Under air-flow navigation (AFN), TIPS pentacene forms thin films with improved crystal orientation and increased areal coverage, which subsequently lead to a four-fold increase of average hole mobility and one order of magnitude enhancement in performance consistency. Chapter 4 investigates the critical roles of lateral and vertical phase separation in the performance of the next-generation organic and hybrid electronic devices. A novel method is demonstrated here to switch between lateral and vertical phase separation in semiconducting TIPS pentacene/ polymer blend films by simply varying the alkyl length of the polyacrylate polymer component. The phase separation modes depend on intermolecular interactions between small molecule TIPS pentacene and polymer additives. The blend film with a dominant vertical phase separation exhibits a significant enhancement in average mobility and performance consistency of organic OTFTs. Chapter 5 demonstrates an effective approach to improve both charge transport and performance consistency in solution-processed OTFTs by blending TIPS pentacene with a series of small-molecule additives: 4-butylbenzoic acid (BBA), 4-hexylbenzoic acid (HBA), and 4-octylbenzoic acid (OBA). These three small molecules share a benzoic acid moiety, but have different length of hydrophobic tails. The self-assembled interfacial layer of small molecules on the gate oxide surface leads to uniform deposition of TIPS pentacene crystal seeds and facilitates TIPS pentacene to grow along the tilted orientation of substrate, which results in a film of enhanced crystal orientation and areal coverage. OTFTs based on TIPS pentacene/small molecule blends demonstrate greatly improved average hole mobility and performance consistency, which correlates with the length of hydrophobic tail of the small-molecule additives. Chapter 6 summarizes the conclusions of this dissertation and the related future work.

Diffusion-controlled growth of molecular heterostructures: fabrication of two-, one-, and zero-dimensional C(60) nanostructures on pentacene substrates.

PubMed

Breuer, Tobias; Witte, Gregor

2013-10-09

A variety of low dimensional C60 structures has been grown on supporting pentacene multilayers. By choice of substrate temperature during growth the effective diffusion length of evaporated fullerenes and their nucleation at terraces or step edges can be precisely controlled. AFM and SEM measurements show that this enables the fabrication of either 2D adlayers or solely 1D chains decorating substrate steps, while at elevated growth temperature continuous wetting of step edges is prohibited and instead the formation of separated C60 clusters pinned at the pentacene step edges occurs. Remarkably, all structures remain thermally stable at room temperature once they are formed. In addition the various fullerene structures have been overgrown by an additional pentacene capping layer. Utilizing the different probe depth of XRD and NEXAFS, we found that no contiguous pentacene film is formed on the 2D C60 structure, whereas an encapsulation of the 1D and 0D structures with uniformly upright oriented pentacene is achieved, hence allowing the fabrication of low dimensional buried organic heterostructures.

Correlation between ambient air and continuous bending stress for the electrical reliability of flexible pentacene-based thin-film transistors

NASA Astrophysics Data System (ADS)

Fan, Ching-Lin; Lin, Wei-Chun; Peng, Han-Hsing; Lin, Yu-Zuo; Huang, Bohr-Ran

2015-01-01

This study investigated how continuous bending stress affects the electrical characteristics of pentacene-based organic thin-film transistors (OTFTs) with poly(4-vinylphenol) (PVP) gate insulator in a vacuum and in ambient air. In tension mode, the strain direction of the fabricated devices was perpendicular to the device channel length. The OTFT devices that were bent in a vacuum exhibited a decreased on current because of cracking in the pentacene channel layer, which can obstruct the transport of charge carriers and deteriorate the on current of the OTFTs. The OTFT devices that were bent in ambient air exhibited a slightly decreased on current and considerably increased off current and subthreshold swing (SS). It was assumed that air moisture passed through the pentacene cracks into the interface between the PVP and pentacene layer, thereby yielding an increase in polar moisture traps, and leading to an increase in the conductivity of the pentacene, thus yielding a slightly decreased on current and considerably increased off current and SS.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Cho, Sang Wan; Lee, Sangho; Kim, Minsoo

The interfacial electronic structure of a bilayer of chloroaluminum phthalocyanine (ClAlPc) and pentacene grown on indium tin oxide (ITO) has been studied using synchrotron-radiation-excited photoelectron spectroscopy. The energy difference between the highest occupied molecular orbital (HOMO) level of the pentacene layer and the lowest unoccupied molecular orbital (LUMO) level of the ClAlPc layer (E HOMO D - E LUMO A ) was determined and compared with that of C 60/pentacene bilayers. The E HOMO D - E LUMO A of a heterojunction with ClAlPc was found to be 1.3 eV while that with C 60 was 0.9 eV. This differencemore » is discussed in terms of the difference in the ionization energy of each acceptor materials. We also obtained the complete energy level diagrams of both ClAlPc/pentacene/ITO and C 60/pentacene/ITO.« less

Electrical characteristics of pentacene-based Schottky diodes

NASA Astrophysics Data System (ADS)

Lee, Y. S.; Park, J. H.; Choi, J. S.

2003-01-01

The current-voltage ( I-V), capacitance-frequency ( C-f), and capacitance-voltage ( C-V) characteristics of organic diodes with a pentacene/aluminum Sckottky contact have been investigated. From the measured diode capacitances, it is revealed that the frequency-dependent properties are related to the localized traps in the band gap of pentacene. The C-V characteristics for different test frequencies are presented. In the low frequency region, the capacitance is nearly constant with reverse bias and increase with the forward bias. With even higher forward bias, the capacitance gradually decreases, which is due to the detrapping of the trapped charges. The intrinsic charge carrier concentration in pentacene was extracted as 3.1×10 17 cm -3 from the C-V characteristics. The C-V properties of the pentacene-based metal-oxide-semiconductor structure have also studied.

Increased mobility and on/off ratio in organic field-effect transistors using low-cost guanine-pentacene multilayers

NASA Astrophysics Data System (ADS)

Shi, Wei; Zheng, Yifan; Taylor, André D.; Yu, Junsheng; Katz, Howard E.

2017-07-01

Layer-by-layer deposited guanine and pentacene in organic field-effect transistors (OFETs) is introduced. Through adjusting the layer thickness ratio of guanine and pentacene, the tradeoff of two electronic parameters in OFETs, charge carrier mobility and current on/off ratio, was controlled. The charge mobility was enhanced by depositing pentacene over and between guanine layers and by increasing the proportion of pentacene in the layer-by-layer system, while the current on/off ratio was increased via the decreased off current induced by the guanine layers. The tunable device performance was mainly ascribed to the trap and dopant neutralizing properties of the guanine layers, which would decrease the density of free hydroxyl groups in the OFETs. Furthermore, the cost of the devices could be reduced remarkably via the adoption of low-cost guanine.

Multiscale Morphology of Organic Semiconductor Thin Films Controls the Adhesion and Viability of Human Neural Cells

PubMed Central

Tonazzini, I.; Bystrenova, E.; Chelli, B.; Greco, P.; Stoliar, P.; Calò, A.; Lazar, A.; Borgatti, F.; D'Angelo, P.; Martini, C.; Biscarini, F.

2010-01-01

Abstract We investigate how multiscale morphology of functional thin films affects the in vitro behavior of human neural astrocytoma 1321N1 cells. Pentacene thin film morphology is precisely controlled by means of the film thickness, Θ (here expressed in monolayers (ML)). Fluorescence and atomic force microscopy allow us to correlate the shape, adhesion, and proliferation of cells to the morphological properties of pentacene films controlled by saturated roughness, σ, correlation length, ξ, and fractal dimension, df. At early incubation times, cell adhesion exhibits a transition from higher to lower values at Θ ≈ 10 ML. This is explained using a model of conformal adhesion of the cell membrane onto the growing pentacene islands. From the model fitting of the data, we show that the cell explores the surface with a deformation of the membrane whose minimum curvature radius is 90 (± 45) nm. The transition in the adhesion at ∼10 ML arises from the saturation of ξ accompanied by the monotonic increase of σ, which leads to a progressive decrease of the pentacene local radius of curvature and hence to the surface area accessible to the cell. Cell proliferation is also enhanced for Θ < 10 ML, and the optimum morphology parameter ranges for cell deployment and growth are σ ≤ 6 nm, ξ > 500 nm, and df > 2.45. The characteristic time of cell proliferation is τ ≈ 10 ± 2 h. PMID:20550892

Increased Coplanarity and Conjugation and Lowered HOMO-LUMO Energy Differences in Benzochalogens Connected to Aromatic Substituents via Ethynyl Spacers: A DFT Study

DTIC Science & Technology

2012-03-25

triisopropylsilylethynyl)- pentacene in which the oxidatively instable 6, 13 positions of pentacene are stabilized by the TIPS groups which also...Table 1. DFT calculations for reference compounds BBT (1), pentacene (6) and 6-αT (7) are listed in Table 2. The structures of molecules 1-7 are shown in...7. Egexp Provides Experimental Data from the Literature HOMO [eV] a LUMO [eV] a Eg [eV] a Egexp [eV] BBT, 1 -5.14 -1.53 3.61 n/a Pentacene , 6

Increased Coplanarity and Conjugation and Lowered HOMO-LUMO Energy Differences in Benzochalogens Connected to Aromatic Substituents via Ethynyl Spacers: A DFT Study

DTIC Science & Technology

2013-03-25

triisopropylsilylethynyl)- pentacene in which the oxidatively instable 6, 13 positions of pentacene are stabilized by the TIPS groups which also...Table 1. DFT calculations for reference compounds BBT (1), pentacene (6) and 6-αT (7) are listed in Table 2. The structures of molecules 1-7 are shown in...7. Egexp Provides Experimental Data from the Literature HOMO [eV] a LUMO [eV] a Eg [eV] a Egexp [eV] BBT, 1 -5.14 -1.53 3.61 n/a Pentacene , 6

Optical Detection and Probing of Single Dopant Molecules of Pentacene in a p-Terphenyl Crystal by Means of Absorption Spectroscopy

DTIC Science & Technology

1989-08-31

Pentacene in a p-Terphenyl Host Crystal bY !eT=s of bsorotion Spectroscopy 12 PERSONAl AU- OR(S) L. Kador, W.E. Moerner & D.E. Horne 1 3a 7 P; OF REPORT...G(OP SUB-GROUP Single Molecule Detection FM Spectroscopy Pentacene in p-terphenyl 19 AtiSTRACT {Continue on reverse it necessary and identity Oy block...OF PENTACENE IN A p-TERPIIENYL IIOST CRYSTAL BY MEANS OF ABSORPTION SPECTROSCOPY L. Kador , 1). E. I lorne, and W. lF. Moerner IM Research )ivision

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tani, Yasuo; Shikoh, Eiji, E-mail: shikoh@elec.eng.osaka-cu.ac.jp; Teki, Yoshio

We report the spin-pump-induced spin transport properties of a pentacene film prepared by thermal evaporation. In a palladium(Pd)/pentacene/Ni{sub 80}Fe{sub 20} tri-layer sample, a pure spin-current is generated in the pentacene layer by the spin-pumping of Ni{sub 80}Fe{sub 20}, which is independent of the conductance mismatch problem in spin injection. The spin current is absorbed into the Pd layer, converted into a charge current with the inverse spin-Hall effect in Pd, and detected as an electromotive force. This is clear evidence for the pure spin current at room temperature in pentacene films prepared by thermal evaporation.

Charge Transfer and Orbital Level Alignment at Inorganic/Organic Interfaces: The Role of Dielectric Interlayers.

PubMed

Hollerer, Michael; Lüftner, Daniel; Hurdax, Philipp; Ules, Thomas; Soubatch, Serguei; Tautz, Frank Stefan; Koller, Georg; Puschnig, Peter; Sterrer, Martin; Ramsey, Michael G

2017-06-27

It is becoming accepted that ultrathin dielectric layers on metals are not merely passive decoupling layers, but can actively influence orbital energy level alignment and charge transfer at interfaces. As such, they can be important in applications ranging from catalysis to organic electronics. However, the details at the molecular level are still under debate. In this study, we present a comprehensive analysis of the phenomenon of charge transfer promoted by a dielectric interlayer with a comparative study of pentacene adsorbed on Ag(001) with and without an ultrathin MgO interlayer. Using scanning tunneling microscopy and photoemission tomography supported by density functional theory, we are able to identify the orbitals involved and quantify the degree of charge transfer in both cases. Fractional charge transfer occurs for pentacene adsorbed on Ag(001), while the presence of the ultrathin MgO interlayer promotes integer charge transfer with the lowest unoccupied molecular orbital transforming into a singly occupied and singly unoccupied state separated by a large gap around the Fermi energy. Our experimental approach allows a direct access to the individual factors governing the energy level alignment and charge-transfer processes for molecular adsorbates on inorganic substrates.

Surface Modification of Solution-Processed ZrO2 Films through Double Coating for Pentacene Thin-Film Transistors

NASA Astrophysics Data System (ADS)

Kwon, Jin-Hyuk; Bae, Jin-Hyuk; Lee, Hyeonju; Park, Jaehoon

2018-03-01

We report the modification of surface properties of solution-processed zirconium oxide (ZrO2) dielectric films achieved by using double-coating process. It is proven that the surface properties of the ZrO2 film are modified through the double-coating process; the surface roughness decreases and the surface energy increases. The present surface modification of the ZrO2 film contributes to an increase in grain size of the pentacene film, thereby increasing the field-effect mobility and decreasing the threshold voltage of the pentacene thin-film transistors (TFTs) having the ZrO2 gate dielectric. Herein, the molecular orientation of pentacene film is also studied based on the results of contact angle and X-ray diffraction measurements. Pentacene molecules on the double-coated ZrO2 film are found to be more tilted than those on the single-coated ZrO2 film, which is attributed to the surface modification of the ZrO2 film. However, no significant differences are observed in insulating properties between the single-and the double-coated ZrO2 dielectric films. Consequently, the characteristic improvements of the pentacene TFTs with the double-coated ZrO2 gate dielectric film can be understood through the increase in pentacene grain size and the reduction in grain boundary density.

Triplet energy transfer and triplet exciton recycling in singlet fission sensitized organic heterojunctions

NASA Astrophysics Data System (ADS)

Hamid, Tasnuva; Yambem, Soniya D.; Crawford, Ross; Roberts, Jonathan; Pandey, Ajay K.

2017-08-01

Singlet exciton fission is a process where an excited singlet state splits into two triplets, thus leading to generation of multiple excitons per absorbed photon in organic semiconductors. Herein, we report a detailed exciton management approach for multiexciton harvesting over a broadband region of the solar spectrum in singlet fission sensitized organic photodiodes. Through systematic studies on the model cascade of pentacene/rubrene/C60, we found that efficient photocurrent generation from pentacene can still occur despite the presence of a >10nm thick interlayer of rubrene in between the pentacene/C60 heterojunction. Our results show that thin rubrene interlayers of thickness < 5 nm are effective in maintaining the delicate balance between two free charge generation channels that progress independently via the electron and hole transfer routes. The contribution to photocurrent from pentacene despite having a reasonably thick rubrene interlayer, that too with higher triplet energy (T1=1.12 eV) than pentacene (T1= 0.86 eV), makes its operation a rather interesting result. We discuss the role of rubrene interlayer film discontinuity, triplet exciton reflection from rubrene interlayer and triplet energy transfer from rubrene to pentacene layer followed by diffusion of triplet excitons through rubrene as plausible mechanisms that would enable triplet excitons from pentacene to generate significant photocurrent in a multilayer organic heterojunction.

Multi-Resolution Imaging of Electron Dynamics in Nanostructure Interfaces

DTIC Science & Technology

2010-07-27

metallic carbon nanotubes from semiconducting ones. In pentacene transistors, we used scanning photocurrent microscopy to study spatially resolved...photoelectric response of pentacene thin films, which showed that point contacts formed near the hole injection points limit the overall performance of the...photothermal current microscopy, carbon nanotube transistor, pentacene transistor, contact resistance, hole injection 16. SECURITY CLASSIFICATION OF

Ambipolar organic thin-film transistor-based nano-floating-gate nonvolatile memory

NASA Astrophysics Data System (ADS)

Han, Jinhua; Wang, Wei; Ying, Jun; Xie, Wenfa

2014-01-01

An ambipolar organic thin-film transistor-based nano-floating-gate nonvolatile memory was demonstrated, with discrete distributed gold nanoparticles, tetratetracontane (TTC), pentacene as the floating-gate layer, tunneling layer, and active layer, respectively. The electron traps at the TTC/pentacene interface were significantly suppressed, which resulted in an ambipolar operation in present memory. As both electrons and holes were supplied in the channel and trapped in the floating-gate by programming/erasing operations, respectively, i.e., one type of charge carriers was used to overwrite the other, trapped, one, a large memory window, extending on both sides of the initial threshold voltage, was realized.

Real-time x-ray scattering study of the initial growth of organic crystals on polymer brushes

DOE Office of Scientific and Technical Information (OSTI.GOV)

An, Sung Yup; Ahn, Kwangseok; Kim, Doris Yangsoo

2014-04-21

We studied the early-stage growth structures of pentacene organic crystals grown on polymer brushes using real-time x-ray scattering techniques. In situ x-ray reflectivity and atomic force microscopy analyses revealed that at temperatures close to the glass transition temperature of polymer brush, the pentacene overlayer on a polymer brush film showed incomplete condensation and 3D island structures from the first monolayer. A growth model based on these observations was used to quantitatively analyze the real-time anti-Bragg x-ray scattering intensities measured during pentacene growth to obtain the time-dependent layer coverage of the individual pentacene monolayers. The extracted total coverage confirmed significant desorptionmore » and incomplete condensation in the pentacene films deposited on the polymer brushes. These effects are ascribed to the change in the surface viscoelasticity of the polymer brushes around the glass transition temperature.« less

Femtosecond stimulated Raman evidence for charge-transfer character in pentacene singlet fission.

PubMed

Hart, Stephanie M; Silva, W Ruchira; Frontiera, Renee R

2018-02-07

Singlet fission is a spin-allowed process in which an excited singlet state evolves into two triplet states. We use femtosecond stimulated Raman spectroscopy, an ultrafast vibrational technique, to follow the molecular structural evolution during singlet fission in order to determine the mechanism of this process. In crystalline pentacene, we observe the formation of an intermediate characterized by pairs of excited state peaks that are red- and blue-shifted relative to the ground state features. We hypothesize that these features arise from the formation of cationic and anionic species due to partial transfer of electron density from one pentacene molecule to a neighboring molecule. These observations provide experimental evidence for the role of states with significant charge-transfer character which facilitate the singlet fission process in pentacene. Our work both provides new insight into the singlet fission mechanism in pentacene and demonstrates the utility of structurally-sensitive time-resolved spectroscopic techniques in monitoring ultrafast processes.

Effect of water layer at the SiO2/graphene interface on pentacene morphology.

PubMed

Chhikara, Manisha; Pavlica, Egon; Matković, Aleksandar; Gajić, Radoš; Bratina, Gvido

2014-10-07

Atomic force microscopy has been used to examine early stages of pentacene growth on exfoliated single-layer graphene transferred to SiO2 substrates. We have observed 2D growth with mean height of 1.5 ± 0.2 nm on as-transferred graphene. Three-dimensional islands of pentacene with an average height of 11 ± 2 nm were observed on graphene that was annealed at 350 °C prior to pentacene growth. Compellingly similar 3D morphology has been observed on graphene transferred onto SiO2 that was treated with hexamethyldisilazane prior to the transfer of graphene. On multilayer graphene we have observed 2D growth, regardless of the treatment of SiO2. We interpret this behavior of pentacene molecules in terms of the influence of the dipolar field that emerges from the water monolayer at the graphene/SiO2 interface on the surface energy of graphene.

A pentacene monolayer trapped between graphene and a substrate.

PubMed

Zhang, Qicheng; Peng, Boyu; Chan, Paddy Kwok Leung; Luo, Zhengtang

2015-09-21

A self-assembled pentacene monolayer can be fabricated between the solid-solid interface of few-layered graphene (FLG) and the mica substrate, through a diffusion-spreading method. By utilizing a transfer method that allows us to sandwich pentacene between graphene and mica, followed by controlled annealing, we enabled the diffused pentacene to be trapped in the interfaces and led to the formation of a stable monolayer. We found that the formation of a monolayer is kinetically favored by using a 2D Ising lattice gas model for pentacene trapped between the graphene-substrate interfaces. This kinetic Monte Carlo simulation results indicate that, due to the graphene substrate enclosure, the spreading of the first layer proceeds faster than the second layer, as the kinetics favors the filling of voids by molecules from the second layer. This graphene assisted monolayer assembly method provides a new avenue for the fabrication of two-dimensional monolayer structures.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nishi, Shohei; Taguchi, Dai; Manaka, Takaaki

By using electric-field-induced optical second-harmonic generation measurement coupled with the conventional current-voltage (I-V) measurement, we studied the carrier transport of organic double-layer diodes with a Au/pentacene/fluorine polymer (FP)/indium zinc oxide (IZO) structure. The rectifying I-V characteristics were converted into the I-E characteristics of the FP and pentacene layers. Results suggest a model in which Schottky-type electron injection from the IZO electrode to the FP layer governs the forward electrical conduction (V > 0), where the space charge electric field produced in the FP layer by accumulated holes at the pentacene/FP interface makes a significant contribution. On the other hand, Schottky-type injection bymore » accumulated interface electrons from the pentacene layer to the FP layer governs the backward electrical conduction (V < 0). The electroluminescence generated from the pentacene layer in the region V > 0 verifies the electron transport across the FP layer, and supports the above suggested model.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yan, Pingrui; Liu, Ziyang; Liu, Dongyang

Pentacene organic thin-film transistors (OTFTs) were prepared by introducing 4, 4″-tris(3-methylphenylphenylamino) triphenylamine (m-MTDATA): MoO{sub 3}, Pentacene: MoO{sub 3}, and Pentacene: m-MTDATA: MoO{sub 3} as buffer layers. These OTFTs all showed significant performance improvement comparing to the reference device. Significantly, we observe that the device employing Pentacene: m-MTDATA: MoO{sub 3} buffer layer can both take advantage of charge transfer complexes formed in the m-MTDATA: MoO{sub 3} device and suitable energy level alignment existed in the Pentacene: MoO{sub 3} device. These two parallel paths led to a high mobility, low threshold voltage, and contact resistance of 0.72 cm{sup 2}/V s, −13.4 V,more » and 0.83 kΩ at V{sub ds} = − 100 V. This work enriches the understanding of MoO{sub 3} doped organic materials for applications in OTFTs.« less

Electrical and Structural Origin of Self-Healing Phenomena in Pentacene Thin Films.

PubMed

Kang, Evan S H; Zhang, Hongbin; Donner, Wolfgang; von Seggern, Heinz

2017-04-01

Self-healing induced by structural phase transformation is demonstrated using pentacene field-effect transistors. During the self-healing process, the electrical properties at the pentacene interfaces improve due to the phase transformation from monolayer phase to thin-film phase. Enhanced mobility is confirmed by first-principles calculations. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Statistical Fine Structure of Inhomogeneously Broadened Absorption Lines.

DTIC Science & Technology

1987-07-31

inhomogeneously broadened optical absorption of pentacene n p-terphenyl at liquid helium temperatures... SFS is the actual frequency- ependent, time...statistical fine structure (SFS) in the inhomogeneously broadened optical absorption of pentacene in p-terphenyl at liquid helium temperatures. SFS is the...quite difficult . -2- We have observed for the first time statistical fine structure in the inhomogeneously broadened optical absorption of pentacene

Laser Physics and Laser Techniques.

DTIC Science & Technology

1980-02-01

excited states is IGNFACTE produced in a pentacene -doped p-terphenyl molecular crystal by SIGNAL optical absorption from two crossed time-coincident...induces coherent microwave acoustic phonons. These in turn modulate, at the sound frequency, the optical absorption properties of the pentacene molecules... pentacene fects in molecular crystals, and particularly the observa- in p-terphenyl has thus been obtained [2]. tion of an acoustooptic amplitude

Molecular gap and energy level diagram for pentacene adsorbed on filled d-band metal surfaces

NASA Astrophysics Data System (ADS)

Baldacchini, Chiara; Mariani, Carlo; Betti, Maria Grazia; Gavioli, L.; Fanetti, M.; Sancrotti, M.

2006-10-01

The authors present a combined photoemission and scanning-tunneling spectroscopy study of the filled electronic states, the molecular energy gap, and the energy level diagram of highly ordered arrays of pentacene deposited on the Cu(119) vicinal surface. The states localized at the interface are clearly singled out, comparing the results at different pentacene thicknesses and with gas-phase photoemission data. The molecular gap of 2.35eV, the hole injection barrier of 1.05eV, and the electron injection barrier of 1.30eV determine the energy level diagram of the states localized at the pentacene molecules.

Pentacene Dimers as a Critical Tool for the Investigation of Intramolecular Singlet Fission.

PubMed

Hetzer, Constantin; Guldi, Dirk M; Tykwinski, Rik R

2018-01-11

Singlet fission (SF) involves the spontaneous splitting of a photoexcited singlet state into a pair of triplets, and it holds great promise toward the realization of more efficient solar cells. Although the process of SF has been known since the 1960s, debate regarding the underlying mechanism continues to this day, especially for molecular materials. A number of different chromophores have been synthesized and studied in order to better understand the process of SF. These previous reports have established that pentacene and its derivatives are especially well-suited for the study of SF, since the energetic requirement E(S 1 )≥2E(T 1 ) is fulfilled rendering the process exothermic and unidirectional. Dimeric pentacene derivatives, in which individual pentacene chromophores are tethered by a "spacer", have emerged as the system of choice toward exploring the mechanism of intramolecular singlet fission (iSF). The dimeric structure, and in particular the spacer, allows for controlling and tuning the distance, geometric relationship, and electronic coupling between the two pentacene moieties. This Minireview describes recent advances using pentacene dimers for the investigation of iSF. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Organic Semiconductors for Sprayable Solar Cells: Improving Stability and Efficiency

DTIC Science & Technology

2008-03-25

adopt a bulk heterojunction approach (where donor and acceptor are mixed before deposition). This decision immediately removed pentacene - based...derivative (ADTz) was the first screened, and unfortunately did not yield any photovoltaic performance. The fullerene adduct of pentacene and C60 was...continue). The most encouraging acceptor was the dicyano pentacene chromophore (DC_Pn). The derivatives shown above varied in efficiency from

Long-Lived Triplet Excited States of Bent-Shaped Pentacene Dimers by Intramolecular Singlet Fission.

PubMed

Sakuma, Takao; Sakai, Hayato; Araki, Yasuyuki; Mori, Tadashi; Wada, Takehiko; Tkachenko, Nikolai V; Hasobe, Taku

2016-03-24

Intramolecular singlet fission (ISF) is a promising photophysical process to construct more efficient light energy conversion systems as one excited singlet state converts into two excited triplet states. Herein we synthesized and evaluated bent-shaped pentacene dimers as a prototype of ISF to reveal intrinsic characters of triplet states (e.g., lifetimes of triplet excited states). In this study, meta-phenylene-bridged TIPS-pentacene dimer (PcD-3Ph) and 2,2'-bipheynyl bridged TIPS-pentacene dimer (PcD-Biph) were newly synthesized as bent-shaped dimers. In the steady-state spectroscopy, absorption and emission bands of these dimers were fully characterized, suggesting the appropriate degree of electronic coupling between pentacene moieties in these dimers. In addition, the electrochemical measurements were also performed to check the electronic interaction between two pentacene moieties. Whereas the successive two oxidation peaks owing to the delocalization were observed in a directly linked-pentacene dimer (PcD) by a single bond, the cyclic voltammograms in PcD-Biph and PcD-3Ph implied the weaker interaction compared to that of p-phenylene-bridged TIPS-pentacene dimer (PcD-4Ph) and PcD. The femtosecond and nanosecond transient absorption spectra clearly revealed the slower ISF process in bent-shaped pentacene dimers (PcD-Biph and PcD-3Ph), more notably, the slower relaxation of the excited triplet states in PcD-Biph and PcD-3Ph. Namely, the quantum yields of triplet states (ΦT) by ISF approximately remain constant (ca. 180-200%) in all dimer systems, whereas the lifetimes of the triplet excited states became much longer (up to 360 ns) in PcD-Biph as compared to PcD-4Ph (15 ns). Additionally, the lifetimes of the corresponding triplet states in PcD-Biph and PcD-3Ph were sufficiently affected by solvent viscosity. In particular, the lifetimes of PcD-Biph triplet state in THF/paraffin (1.0 μs) increased up to approximately three times as compared to that in THF (360 ns), whereas those of PcD-4Ph were quite similar in both solvent.

Structure and transport in organic semiconductor thin films

NASA Astrophysics Data System (ADS)

Vos, Sandra Elizabeth Fritz

Organic Semiconductors represent an exciting area of research due to their potential application in cheap and flexible electronics. In spite of the abundant interest in organic electronics the electronic transport mechanism remains poorly understood. Understanding the connection between molecular structure, crystal packing, intermolecular interactions and electronic delocalization is an important aspect of improving the transport properties of organics in thin film transistors (TFTs). In an organic thin film transistor, charge carrier transport is believed to occur within the first few monolayers of the organic material adjacent to the dielectric. It is therefore critical to understand the initial stages of film growth and molecular structure in these first few layers and relate this structure to electronic transport properties. The structure of organic films at the interface with an amorphous silicon dioxide ( a-SiO2) dielectric and how structure relates to transport in a TFT is the focus of this thesis. Pentacene films on a-SiO2 were extensively characterized with specular and in-plane X-ray diffraction, and CuKalpha1, and synchrotron radiation. The first layer of pentacene molecules adjacent to the a-SiO2 crystallized in a rectangular unit cell with the long axis of the molecules perpendicular to the substrate surface. Subsequent layers of pentacene crystallized in a slightly oblique in-plane unit cell that evolved as thickness was increased. The rectangular monolayer phase of pentacene did not persist when subsequent layers were deposited. Specular diffraction with Synchrotron radiation of a 160 A pentacene film (˜ 10 layers) revealed growth initiation of a bulk-like phase and persistence of the thin-film phase. Pentacene molecules were more tilted in the bulk-like phase and the in-plane unit cell was slightly more oblique. Pentacene grains began to grow randomly oriented with respect to the substrate surface (out-of-plane) in films near 650 A in thickness. The single crystal bulk phase of pentacene was observed from specular diffraction (CuKalpha1) of a 2.5 mum film. These results suggest that the thickness of pentacene films on a-SiO2 is an important aspect in the comparison of crystal structure and electronic transport.

Hybrid, Gate-Tunable, van der Waals p–n Heterojunctions from Pentacene and MoS 2

DOE PAGES

Jariwala, Deep; Howell, Sarah L.; Chen, Kan-Sheng; ...

2015-12-18

The recent emergence of a wide variety of two-dimensional (2D) materials has created new opportunities for device concepts and applications. In particular, the availability of semiconducting transition metal dichalcogenides, in addition to semimetallic graphene and insulating boron nitride, has enabled the fabrication of “all 2D” van der Waals heterostructure devices. Furthermore, the concept of van der Waals heterostructures has the potential to be significantly broadened beyond layered solids. For example, molecular and polymeric organic solids, whose surface atoms possess saturated bonds, are also known to interact via van der Waals forces and thus offer an alternative for scalable integration withmore » 2D materials. Here, we demonstrate the integration of an organic small molecule p-type semiconductor, pentacene, with a 2D n-type semiconductor, MoS2. The resulting p–n heterojunction is gate-tunable and shows asymmetric control over the antiambipolar transfer characteristic. In addition, the pentacene/MoS2 heterojunction exhibits a photovoltaic effect attributable to type II band alignment, which suggests that MoS2 can function as an acceptor in hybrid solar cells.« less

Hybrid, Gate-Tunable, van der Waals p–n Heterojunctions from Pentacene and MoS 2

DOE PAGES

Jariwala, Deep; Howell, Sarah L.; Chen, Kan -Sheng; ...

2015-12-10

Here, the recent emergence of a wide variety of two-dimensional (2D) materials has created new opportunities for device concepts and applications. In particular, the availability of semiconducting transition metal dichalcogenides, in addition to semimetallic graphene and insulating boron nitride, has enabled the fabrication of “all 2D” van der Waals heterostructure devices. Furthermore, the concept of van der Waals heterostructures has the potential to be significantly broadened beyond layered solids. For example, molecular and polymeric organic solids, whose surface atoms possess saturated bonds, are also known to interact via van der Waals forces and thus offer an alternative for scalable integrationmore » with 2D materials. Here, we demonstrate the integration of an organic small molecule p-type semiconductor, pentacene, with a 2D n-type semiconductor, MoS 2. The resulting p–n heterojunction is gate-tunable and shows asymmetric control over the antiambipolar transfer characteristic. In addition, the pentacene/MoS 2 heterojunction exhibits a photovoltaic effect attributable to type II band alignment, which suggests that MoS 2 can function as an acceptor in hybrid solar cells.« less

Hybrid, Gate-Tunable, van der Waals p–n Heterojunctions from Pentacene and MoS 2

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jariwala, Deep; Howell, Sarah L.; Chen, Kan -Sheng

Here, the recent emergence of a wide variety of two-dimensional (2D) materials has created new opportunities for device concepts and applications. In particular, the availability of semiconducting transition metal dichalcogenides, in addition to semimetallic graphene and insulating boron nitride, has enabled the fabrication of “all 2D” van der Waals heterostructure devices. Furthermore, the concept of van der Waals heterostructures has the potential to be significantly broadened beyond layered solids. For example, molecular and polymeric organic solids, whose surface atoms possess saturated bonds, are also known to interact via van der Waals forces and thus offer an alternative for scalable integrationmore » with 2D materials. Here, we demonstrate the integration of an organic small molecule p-type semiconductor, pentacene, with a 2D n-type semiconductor, MoS 2. The resulting p–n heterojunction is gate-tunable and shows asymmetric control over the antiambipolar transfer characteristic. In addition, the pentacene/MoS 2 heterojunction exhibits a photovoltaic effect attributable to type II band alignment, which suggests that MoS 2 can function as an acceptor in hybrid solar cells.« less

Influences of semiconductor morphology on the mechanical fatigue behavior of flexible organic electronics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, Young-Joo; Yeon, Han-Wool; Shin, Hae-A-Seul

2013-12-09

The influence of crystalline morphology on the mechanical fatigue of organic semiconductors (OSCs) was investigated using 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene) as a crystalline OSC and poly(triarylamine) (PTAA) as an amorphous OSC. During cyclic bending, resistances of the OSCs were monitored using the transmission-line method on a metal-semiconductor-metal structure. The resistance of the TIPS-pentacene increased under fatigue damage in tensile-stress mode, but no such degradation was observed in the PTAA. Both OSCs were stable under compressive bending fatigue. The formation of intergranular cracks at the domain boundaries of the TIPS-pentacene was responsible for the degradation of its electrical properties under tensile bending fatigue.

Aryl substitution of pentacenes

PubMed Central

Waterloo, Andreas R; Sale, Anna-Chiara; Lehnherr, Dan; Hampel, Frank

2014-01-01

Summary A series of 11 new pentacene derivatives has been synthesized, with unsymmetrical substitution based on a trialkylsilylethynyl group at the 6-position and various aryl groups appended to the 13-position. The electronic and physical properties of the new pentacene chromophores have been analyzed by UV–vis spectroscopy (solution and thin films), thermoanalytical methods (DSC and TGA), cyclic voltammetry, as well as X-ray crystallography (for 8 derivatives). X-ray crystallography has been specifically used to study the influence of unsymmetrical substitution on the solid-state packing of the pentacene derivatives. The obtained results add to our ability to better predict substitution patterns that might be helpful for designing new semiconductors for use in solid-state devices. PMID:25161729

Nonvolatile floating gate organic memory device based on pentacene/CdSe quantum dot heterojuction

NASA Astrophysics Data System (ADS)

Shin, Ik-Soo; Kim, Jung-Min; Jeun, Jun-Ho; Yoo, Seok-Hyun; Ge, Ziyi; Hong, Jong-In; Ho Bang, Jin; Kim, Yong-Sang

2012-04-01

An organic floating-gate memory device using CdSe quantum dots (QDs) as a charge-trapping element was fabricated. CdSe QDs were localized beneath a pentacene without any tunneling insulator, and the QD layer played a role as hole-trapping sites. The band bending formed at the junction between pentacene and QD layers inhibited back-injection of holes trapped in CdSe into pentacene, which appeared as a hysteretic capacitance-voltage response during the operation of the device. Nearly, 60% of trapped charge was sustained even after 104 s in programmed state, and this long retention time can be potentially useful in practical applications of non-volatile memory.

Hysteresis mechanism and control in pentacene organic field-effect transistors with polymer dielectric

NASA Astrophysics Data System (ADS)

Huang, Wei; Shi, Wei; Han, Shijiao; Yu, Junsheng

2013-05-01

Hysteresis mechanism of pentacene organic field-effect transistors (OFETs) with polyvinyl alcohol (PVA) and/or polymethyl methacrylate (PMMA) dielectrics is studied. Through analyzing the electrical characteristics of OFETs with various PVA/PMMA arrangements, it shows that charge, which is trapped in PVA bulk and at the interface of pentacene/PVA, is one of the origins of hysteresis. The results also show that memory window is proportional to both trap amount in PVA and charge density at the gate/PVA or PVA/pentacene interfaces. Hence, the controllable memory window of around 0 ˜ 10 V can be realized by controlling the thickness and combination of triple-layer polymer dielectrics.

Spectral resolution of states relevant to photoinduced charge transfer in modified pentacene/ZnO field-effect transistors

NASA Astrophysics Data System (ADS)

Spalenka, Josef W.; Mannebach, Ehren M.; Bindl, Dominick J.; Arnold, Michael S.; Evans, Paul G.

2011-11-01

Pentacene field-effect transistors incorporating ZnO quantum dots can be used as a sensitive probe of the optical properties of a buried donor-acceptor interface. Photoinduced charge transfer between pentacene and ZnO in these devices varies with incident photon energy and reveals which energies will contribute most to charge transfer in other structures. A subsequent slow return to the dark state following the end of illumination arises from near-interface traps. Charge transfer has a sharp onset at 1.7 eV and peaks at 1.82 and 2.1 eV due to transitions associated with excitons, features absent in pentacene FETs without ZnO.

Photoresponse and photo-induced memory effect in the organic field-effect transistor based on AlOX nanoparticles at the interface of semiconductor/dielectric

NASA Astrophysics Data System (ADS)

Cheng, Yunfei; Wang, Wu

2017-10-01

In this work, the photoresponse and photo-induced memory effect were demonstrated in an organic field-effect transistor (OFET) with semiconductor pentacene and SiO2 as the active and gate dielectric layers, respectively. By inserting AlOX nanoparticles (NPs) at the interface of pentacene/SiO2, obvious enhancing photoresponse was obtained in the OFET with the maximum responsivity and photosensitivity of about 15 A/W and 100, respectively. Moreover, the stable photoinduced memory effect was achieved in the OFET, attributing to the photogenerated electrons captured by the interface traps of the AlOX NPs/SiO2.

Remarkable reduction in the threshold voltage of pentacene-based thin film transistors with pentacene/CuPc sandwich configuration

NASA Astrophysics Data System (ADS)

Li, Yi; Liu, Qi; Cai, Jing; Li, Yun; Shi, Yi; Wang, Xizhang; Hu, Zheng

2014-06-01

This study investigates the remarkable reduction in the threshold voltage (VT) of pentacene-based thin film transistors with pentacene/copper phthalocyanine (CuPc) sandwich configuration. This reduction is accompanied by increased mobility and lowered sub-threshold slope (S). Sandwich devices coated with a 5 nm layer of CuPc layer are compared with conventional top-contact devices, and results indicate that VT decreased significantly from -20.4 V to -0.2 V, that mobility increased from 0.18 cm2/Vs to 0.51 cm2/Vs, and that S was reduced from 4.1 V/dec to 2.9 V/dec. However, the on/off current ratio remains at 105. This enhanced performance could be attributed to the reduction in charge trap density by the incorporated CuPc layer. Results suggest that this method is simple and effectively generates pentacene-based organic thin film transistors with high mobility and low VT.

Effect of interface-dependent crystalline boundary on sub-threshold characteristics in a solution-processed 6,13-bis(triisopropylsilylethynyl)-pentacene thin-film transistor

NASA Astrophysics Data System (ADS)

Kwon, Jin-Hyuk; Kang, In Man; Bae, Jin-Hyuk

2014-03-01

We demonstrate how the sub-threshold characteristics are affected by the density of crystalline domain boundaries directly governed by an organic semiconductor (OSC) - a gate insulator interface in a solution-processed 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS-pentacene) thin-film transistor (TFT). For generation of an engineered interface, a self assembled monolayer of octadecyltricholorosilane (OTS) was produced between a solution processed TIPS-pentacene film and a silicon dioxide layer. The interfacial charge trap density (Ntrap) deduced from the sub-threshold characteristics was significantly minimized after OTS treatment due to reduced crystal domain boundaries in the TIPS-pentacene film. In addition, the carrier mobility exhibits a value twice as large by OTS treatment. It is found that less crystal domain boundaries in the solution-processed OSC obtained from the engineered interface play an important role in inducing improved sub-threshold characteristics together with increased carrier mobility in organic TFTs.

Ultrasensitive Laser Spectroscopy in Solids: Statistical Fine Structure and Single-Molecule Detection

DTIC Science & Technology

1990-03-28

observation, detection of the optical absorption of a single pentacene molecule in a p-terphenyl crystal, opens the door to new studies of single local ...produce appreciable quadratic Stark shifting. Such effects would greatly perturb the local field around the pentacene molecule, making detection of the...of the local surroundings of pentacene molecules with single injected charge carriers nearby may become an interesting field; however, for the

Structural Design and Photochemical Preparation of Ultrathin Molecular Film Materials

DTIC Science & Technology

2006-12-01

tetracene and pentacene that have great potential as organic semiconducting materials, have been determined. Overall, we have gained to great extend a...layer of linear acenes, molecules such as tetracene and pentacene that have great potential as organic semiconducting materials, have been determined...intermolecular interaction of mono- and multi-layer linear acenes on metal A systematic study of adsorption of linear acenes, from benzene to pentacene , on metal

Single Molecule Spectral Diffusion in a Solid Detected Via Fluorescence Spectroscopy

DTIC Science & Technology

1991-10-15

other local fields) at the position of the molecule, the spectral jumps may occur because the class II pentacene molecules are coupled to an...and identify by block number) FIELD jGROUP SUB-GROUP_ Single molecule spectroscopy Precision detection Spectral diffusion, Pentacene in p-terphenyl 19...significant increases in detection sensitivity for single pentacene molecules in crystals of p-terphenyl at low temperatures. With the increased signal to

Optical Modification of a Single Impurity Molecule in a Solid

DTIC Science & Technology

1991-10-17

have led to direct observations of the lifetime-limited homogeneous Iinewidth of a single pentacene molecule as well as the surprising observation of...advances in the optical detection and spectroscopy of single impurity centers in solids. For the system composed of pentacene impurity molecules in the...limited homogcncous linewidth of a single pentacene molecule as well as the surprising observation of spontaneous spectral diffusion in a crystal

Novel top-contact monolayer pentacene-based thin-film transistor for ammonia gas detection.

PubMed

Mirza, Misbah; Wang, Jiawei; Li, Dexing; Arabi, S Atika; Jiang, Chao

2014-04-23

We report on the fabrication of an organic field-effect transistor (OFET) of a monolayer pentacene thin film with top-contact electrodes for the aim of ammonia (NH3) gas detection by monitoring changes in its drain current. A top-contact configuration, in which source and drain electrodes on a flexible stamp [poly(dimethylsiloxane)] were directly contacted with the monolayer pentacene film, was applied to maintain pentacene arrangement ordering and enhance the monolayer OFET detection performance. After exposure to NH3 gas, the carrier mobility at the monolayer OFET channel decreased down to one-third of its original value, leading to a several orders of magnitude decrease in the drain current, which tremendously enhanced the gas detection sensitivity. This sensitivity enhancement to a limit of the 10 ppm level was attributed to an increase of charge trapping in the carrier channel, and the amount of trapped states was experimentally evaluated by the threshold voltage shift induced by the absorbed NH3 molecular analyte. In contrast, a conventional device with a 50-nm-thick pentacene layer displayed much higher mobility but lower response to NH3 gas, arising from the impediment of analyte penetrating into the conductive channel, owing to the thick pentacene film.

Femtosecond stimulated Raman evidence for charge-transfer character in pentacene singlet fission† †Electronic supplementary information (ESI) available: Actinic pump spectrum, discussion on ground state addition process, peak fitting procedure, transient absorption data, power dependence measurements, etalon pulse shaping, TIPS-pentacene FSRS data, and optimized geometry and frequency calculation results. See DOI: 10.1039/c7sc03496b

PubMed Central

Hart, Stephanie M.; Silva, W. Ruchira

2017-01-01

Singlet fission is a spin-allowed process in which an excited singlet state evolves into two triplet states. We use femtosecond stimulated Raman spectroscopy, an ultrafast vibrational technique, to follow the molecular structural evolution during singlet fission in order to determine the mechanism of this process. In crystalline pentacene, we observe the formation of an intermediate characterized by pairs of excited state peaks that are red- and blue-shifted relative to the ground state features. We hypothesize that these features arise from the formation of cationic and anionic species due to partial transfer of electron density from one pentacene molecule to a neighboring molecule. These observations provide experimental evidence for the role of states with significant charge-transfer character which facilitate the singlet fission process in pentacene. Our work both provides new insight into the singlet fission mechanism in pentacene and demonstrates the utility of structurally-sensitive time-resolved spectroscopic techniques in monitoring ultrafast processes. PMID:29675170

Polymer-Oxide Nanolayer/Al Composite Cathode for Efficient Polymer Light-Emitting Diodes

DTIC Science & Technology

2007-06-30

4. Influence of polymer gate dielectrics on n-channel conduction of pentacene -based organic field-effect transistors J. Appl. Phys. 101, 124505...molecular materials, including rubrene, 1,3,5-tris(2-N-phenyl-benzimidzolyl)benzene (TPBI), pentacene , and 2,9-dimethyl-4,7-diphenyl-1,10-phenanthroline...BCP, and pentacene . The inset in Fig. 3 presents the molecular structures. TPBI is often utilized as an effective electron injection and hole-blocking

Evidence for charge-trapping inducing polymorphic structural-phase transition in pentacene.

PubMed

Ando, Masahiko; Kehoe, Tom B; Yoneya, Makoto; Ishii, Hiroyuki; Kawasaki, Masahiro; Duffy, Claudia M; Minakata, Takashi; Phillips, Richard T; Sirringhaus, Henning

2015-01-07

Trapped-charge-induced transformation of pentacene polymorphs is observed by using in situ Raman spectroscopy and molecular dynamics simulations reveal that the charge should be localized in pentacene molecules at the interface with static intermolecular disorder along the long axis. Quantum chemical calculations of the intermolecular transfer integrals suggest the disorder to be large enough to induce Anderson-type localization. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fabrication of High-Performance Polymer Bulk-Heterojunction Solar Cells by the Interfacial Modifications III

DTIC Science & Technology

2011-04-30

University of Tennessee) 3. "An ambipolar to n-type transformation in pentacene -based organic field-effect transistors" Org. Electron. 12, 509 (2011...OFETs). An ambipolar to n-type transformation in pentacene -based organic field-effect transistors (OFETs) of Al source-drain electrodes had been...correlated with the interfacial interactions between Al electrodes and pentacene , as characterized by analyzing Near-edge X-ray absorption fine structure

Gate-dependent asymmetric transport characteristics in pentacene barristors with graphene electrodes.

PubMed

Hwang, Wang-Taek; Min, Misook; Jeong, Hyunhak; Kim, Dongku; Jang, Jingon; Yoo, Daekyung; Jang, Yeonsik; Kim, Jun-Woo; Yoon, Jiyoung; Chung, Seungjun; Yi, Gyu-Chul; Lee, Hyoyoung; Wang, Gunuk; Lee, Takhee

2016-11-25

We investigated the electrical characteristics and the charge transport mechanism of pentacene vertical hetero-structures with graphene electrodes. The devices are composed of vertical stacks of silicon, silicon dioxide, graphene, pentacene, and gold. These vertical heterojunctions exhibited distinct transport characteristics depending on the applied bias direction, which originates from different electrode contacts (graphene and gold contacts) to the pentacene layer. These asymmetric contacts cause a current rectification and current modulation induced by the gate field-dependent bias direction. We observed a change in the charge injection barrier during variable-temperature current-voltage characterization, and we also observed that two distinct charge transport channels (thermionic emission and Poole-Frenkel effect) worked in the junctions, which was dependent on the bias magnitude.

Epitaxial Growth of an Organic p-n Heterojunction: C60 on Single-Crystal Pentacene.

PubMed

Nakayama, Yasuo; Mizuno, Yuta; Hosokai, Takuya; Koganezawa, Tomoyuki; Tsuruta, Ryohei; Hinderhofer, Alexander; Gerlach, Alexander; Broch, Katharina; Belova, Valentina; Frank, Heiko; Yamamoto, Masayuki; Niederhausen, Jens; Glowatzki, Hendrik; Rabe, Jürgen P; Koch, Norbert; Ishii, Hisao; Schreiber, Frank; Ueno, Nobuo

2016-06-01

Designing molecular p-n heterojunction structures, i.e., electron donor-acceptor contacts, is one of the central challenges for further development of organic electronic devices. In the present study, a well-defined p-n heterojunction of two representative molecular semiconductors, pentacene and C60, formed on the single-crystal surface of pentacene is precisely investigated in terms of its growth behavior and crystallographic structure. C60 assembles into a (111)-oriented face-centered-cubic crystal structure with a specific epitaxial orientation on the (001) surface of the pentacene single crystal. The present experimental findings provide molecular scale insights into the formation mechanisms of the organic p-n heterojunction through an accurate structural analysis of the single-crystalline molecular contact.

Adsorption of pentacene on (100) vicinal surfaces: role of coordination, surface chemistry and vdWs effects

NASA Astrophysics Data System (ADS)

Matos, Jeronimo; Kara, Abdelkader

2015-03-01

In contrast to low miller index surfaces, vicinal surfaces are characterized by steps and step edges that not only present an interesting atomic landscape for the adsorption organic molecules, but also a unique electronic structure resulting in part from the low coordinated atoms at the step edges. The adsorption of pentacene on the stepped (511), (711), (911) surfaces (respectively 3, 4 and 5-atom wide terraces) of Cu and Ag (coinage transition metals); Pt (reactive transition metal); and Ni (reactive, magnetic transition metal) are studied using density functional theory, in order to investigate the support effects arising from differing surface chemistry. We compare the adsorption energy, adsorption geometry and electronic structure predicted by the PBE functional with those obtained from one of the optimized vdW-DF methods: optB88-vdW. Work supported by the U.S. Department of Energy Basic Energy Science under Contract No. DE-FG02-11ER16243.

Composite films of oxidized multiwall carbon nanotube and poly(3,4-ethylenedioxythiophene): polystyrene sulfonate (PEDOT:PSS) as a contact electrode for transistor and inverter devices.

PubMed

Yun, Dong-Jin; Rhee, Shi-Woo

2012-02-01

Composite films of multiwall carbon nanotube (MWNT)/poly(3,4-ethylenedioxythiophene) polymerized with poly(4-styrenesulfonate) (PEDOT:PSS) were prepared by spin-coating a mixture solution. The effect of the MWNT loading and the MWNT oxidation, with acid solution or ultraviolet (UV)-ozone treatment, on the film properties such as surface roughness, work function, surface energy, optical transparency and conductivity were studied. Also pentacene thin film transistors and inverters were made with these composite films as a contact metal and the device characteristics were measured. The oxidation of MWNT reduced the conductivity of MWNT/PEDOT:PSS composite film but increased the work function and transparency. UV-ozone treated MWNT/PEDOT:PSS composite film showed higher conductivity (14000 Ω/□) and work function (4.9 eV) than acid-oxidized MWNT/PEDOT:PSS composite film and showed better performance as a source/drain electrode in organic thin film transistor (OTFT) than other types of MWNT/PEDOT:PSS composite films. Hole injection barrier of the UV-ozone treated MWNT/PEDOT:PSS composite film with pentacene was significantly lower than any other films because of the higher work function.

Effects of molecular packing in organic crystals on singlet fission with ab initio many body perturbation theory

NASA Astrophysics Data System (ADS)

Haber, Jonah; Refaely-Abramson, Sivan; da Jornada, Felipe H.; Louie, Steven G.; Neaton, Jeffrey B.

Multi-exciton generation processes, in which multiple charge carriers are generated from a single photon, are mechanisms of significant interest for achieving efficiencies beyond the Shockley-Queisser limit of conventional p-n junction solar cells. One well-studied multiexciton process is singlet fission, whereby a singlet decays into two spin-correlated triplet excitons. Here, we use a newly developed computational approach to calculate singlet-fission coupling terms and rates with an ab initio Green's function formalism based on many-body perturbation theory (MBPT) within the GW approximation and the Bethe-Salpeter equation approach. We compare results for crystalline pentacene and TIPS-pentacene and explore the effect of molecular packing on the singlet fission mechanism. This work is supported by the Department of Energy.

Optical Probe of the Density of Defect States in Organic Thin-Film Transistors

NASA Astrophysics Data System (ADS)

Breban, Mihaela; Romero, Danilo; Ballarotto, Vincent; Williams, Ellen

2006-03-01

We investigate the role of defect states associated with different gate dielectric materials on charge transport in organic thin film transistors. Using a modulation technique we measure the magnitude and the phase of the photocurrent^1 in pentacene thin film transistors as a function of the modulation frequency. The photocurrent generation process is modeled as exciton dissociation due to interaction with localized traps. A time domain analyses of this multi-step process allows us to extract the density of defect states. We use this technique to compare the physical mechanism underlying performances of pentacene devices fabricated with different dielectric materials. *Supported by the Laboratory for Physical Science ^1 M. Breban, et al. ``Photocurrent probe of field-dependent mobility in organic thin-film transistors'' Appl. Phys. Letts. 87, 203503 (2005)

Pentacene Organic Thin-Film Transistors on Flexible Paper and Glass Substrates

DTIC Science & Technology

2014-02-12

FEB 2014 2. REPORT TYPE 3. DATES COVERED 00-00-2014 to 00-00-2014 4. TITLE AND SUBTITLE Pentacene organic thin - film transistors on flexible...Nanotechnology 25 (2014) 094005 (7pp) doi:10.1088/0957-4484/25/9/094005 Pentacene organic thin - film transistors on flexible paper and glass substrates Adam T...organic thin - film transistors (OTFTs) were fabricated on several types of flexible substrate: commercial photo paper, ultra-smooth specialty paper and

Finding a Single Molecule in a Haystack: Optical Detection and Spectroscopy of Single Absorbers in Solids

DTIC Science & Technology

1989-08-18

CODES 18 SUBJECT TERMS (Continue on reverse if necessary and identify by block number) FIELD GROUP SUB-GROUP Single Molecule Detection Pentacene in p...and 10 additional pentacene molecules. This may be accomplished by- a combination of laser FM spectroscopy and either Stark or ultrasonic double...6099 408-927-2426 ABSTRACT: Single-absorber optical spectroscopy in solids is described for the case of finding a single pentacene molecule in a

Mapping of trap densities and hotspots in pentacene thin-film transistors by frequency-resolved scanning photoresponse microscopy.

PubMed

Westermeier, Christian; Fiebig, Matthias; Nickel, Bert

2013-10-25

Frequency-resolved scanning photoresponse microscopy of pentacene thin-film transistors is reported. The photoresponse pattern maps the in-plane distribution of trap states which is superimposed by the level of trap filling adjusted by the gate voltage of the transistor. Local hotspots in the photoresponse map thus indicate areas of high trap densities within the pentacene thin film. © 2013 WILEY-VCH Verlag GmbH 8 Co. KGaA, Weinheim.

Molecular Self-Assembly and Interfacial Engineering for Highly Efficient Organic Field Effect Transistors and Solar Cells

DTIC Science & Technology

2012-09-23

balance between disordered SAMs to promote large pentacene grains and thick SAMs to aid in physically buffering the charge carriers in pentacene from...to 0.76 µF/cm2), and enhanced pentacene OFET device performance such as higher charge carrier mobility, current on/off ratio, and lower threshold...surface charge trap • Tuning of surface energy • Control of surface group orientation SAM/MO ultrathin dielectric: • Low-voltage operation

Effects of self-assembled monolayer structural order, surface homogeneity and surface energy on pentacene morphology and thin film transistor device performance.

PubMed

Hutchins, Daniel Orrin; Weidner, Tobias; Baio, Joe; Polishak, Brent; Acton, Orb; Cernetic, Nathan; Ma, Hong; Jen, Alex K-Y

2013-01-04

A systematic study of six phosphonic acid (PA) self-assembled monolayers (SAMs) with tailored molecular structures is performed to evaluate their effectiveness as dielectric modifying layers in organic field-effect transistors (OFETs) and determine the relationship between SAM structural order, surface homogeneity, and surface energy in dictating device performance. SAM structures and surface properties are examined by near edge X-ray absorption fine structure (NEXAFS) spectroscopy, contact angle goniometry, and atomic force microscopy (AFM). Top-contact pentacene OFET devices are fabricated on SAM modified Si with a thermally grown oxide layer as a dielectric. For less ordered methyl- and phenyl-terminated alkyl ~(CH 2 ) 12 PA SAMs of varying surface energies, pentacene OFETs show high charge carrier mobilities up to 4.1 cm 2 V -1 s -1 . It is hypothesized that for these SAMs, mitigation of molecular scale roughness and subsequent control of surface homogeneity allow for large pentacene grain growth leading to high performance pentacene OFET devices. PA SAMs that contain bulky terminal groups or are highly crystalline in nature do not allow for a homogenous surface at a molecular level and result in charge carrier mobilities of 1.3 cm 2 V -1 s -1 or less. For all molecules used in this study, no causal relationship between SAM surface energy and charge carrier mobility in pentacene FET devices is observed.

Ultrafast Exciton Dissociation and Long-Lived Charge Separation in a Photovoltaic Pentacene-MoS2 van der Waals Heterojunction.

PubMed

Bettis Homan, Stephanie; Sangwan, Vinod K; Balla, Itamar; Bergeron, Hadallia; Weiss, Emily A; Hersam, Mark C

2017-01-11

van der Waals heterojunctions between two-dimensional (2D) layered materials and nanomaterials of different dimensions present unique opportunities for gate-tunable optoelectronic devices. Mixed-dimensional p-n heterojunction diodes, such as p-type pentacene (0D) and n-type monolayer MoS 2 (2D), are especially interesting for photovoltaic applications where the absorption cross-section and charge transfer processes can be tailored by rational selection from the vast library of organic molecules and 2D materials. Here, we study the kinetics of excited carriers in pentacene-MoS 2 p-n type-II heterojunctions by transient absorption spectroscopy. These measurements show that the dissociation of MoS 2 excitons occurs by hole transfer to pentacene on the time scale of 6.7 ps. In addition, the charge-separated state lives for 5.1 ns, up to an order of magnitude longer than the recombination lifetimes from previously reported 2D material heterojunctions. By studying the fractional amplitudes of the MoS 2 decay processes, the hole transfer yield from MoS 2 to pentacene is found to be ∼50%, with the remaining holes undergoing trapping due to surface defects. Overall, the ultrafast charge transfer and long-lived charge-separated state in pentacene-MoS 2 p-n heterojunctions suggest significant promise for mixed-dimensional van der Waals heterostructures in photovoltaics, photodetectors, and related optoelectronic technologies.

Blending effect of 6,13-bis(triisopropylsilylethynyl) pentacene-graphene composite layers for flexible thin film transistors with a polymer gate dielectric.

PubMed

Basu, Sarbani; Adriyanto, Feri; Wang, Yeong-Her

2014-02-28

Solution processible poly(4-vinylphenol) is employed as a transistor dielectric material for low cost processing on flexible substrates at low temperatures. A 6,13-bis (triisopropylsilylethynyl) (TIPS) pentacene-graphene hybrid semiconductor is drop cast to fabricate bottom-gate and bottom-contact field-effect transistor devices on flexible and glass substrates under an ambient air environment. A few layers of graphene flakes increase the area in the conduction channel, and form bridge connections between the crystalline regions of the semiconductor layer which can change the surface morphology of TIPS pentacene films. The TIPS pentacene-graphene hybrid semiconductor-based organic thin film transistors (OTFTs) cross-linked with a poly(4-vinylphenol) gate dielectric exhibit an effective field-effect mobility of 0.076 cm(2) V(-1) s(-1) and a threshold voltage of -0.7 V at V(gs) = -40 V. By contrast, typical TIPS pentacene shows four times lower mobility of 0.019 cm(2) V(-1) s(-1) and a threshold voltage of 5 V. The graphene/TIPS pentacene hybrids presented in this paper can enhance the electrical characteristics of OTFTs due to their high crystallinity, uniform large-grain distribution, and effective reduction of crystal misorientation of the organic semiconductor layer, as confirmed by x-ray diffraction spectroscopy, atomic force microscopy, and optical microscopy studies.

Effects of self-assembled monolayer structural order, surface homogeneity and surface energy on pentacene morphology and thin film transistor device performance

PubMed Central

Hutchins, Daniel Orrin; Weidner, Tobias; Baio, Joe; Polishak, Brent; Acton, Orb; Cernetic, Nathan; Ma, Hong; Jen, Alex K.-Y.

2013-01-01

A systematic study of six phosphonic acid (PA) self-assembled monolayers (SAMs) with tailored molecular structures is performed to evaluate their effectiveness as dielectric modifying layers in organic field-effect transistors (OFETs) and determine the relationship between SAM structural order, surface homogeneity, and surface energy in dictating device performance. SAM structures and surface properties are examined by near edge X-ray absorption fine structure (NEXAFS) spectroscopy, contact angle goniometry, and atomic force microscopy (AFM). Top-contact pentacene OFET devices are fabricated on SAM modified Si with a thermally grown oxide layer as a dielectric. For less ordered methyl- and phenyl-terminated alkyl ~(CH2)12 PA SAMs of varying surface energies, pentacene OFETs show high charge carrier mobilities up to 4.1 cm2 V−1 s−1. It is hypothesized that for these SAMs, mitigation of molecular scale roughness and subsequent control of surface homogeneity allow for large pentacene grain growth leading to high performance pentacene OFET devices. PA SAMs that contain bulky terminal groups or are highly crystalline in nature do not allow for a homogenous surface at a molecular level and result in charge carrier mobilities of 1.3 cm2 V−1 s−1 or less. For all molecules used in this study, no causal relationship between SAM surface energy and charge carrier mobility in pentacene FET devices is observed. PMID:24086795

Molecular dynamics simulations of graphoepitaxy of organic semiconductors, sexithiophene, and pentacene: Molecular-scale mechanisms of organic graphoepitaxy

NASA Astrophysics Data System (ADS)

Ikeda, Susumu

2018-03-01

Molecular dynamics (MD) simulations of the organic semiconductors α-sexithiophene (6T) and pentacene were carried out to clarify the mechanism of organic graphoepitaxy at the molecular level. First, the models of the grooved substrates were made and the surfaces of the inside of the grooves were modified with -OH or -OSi(CH3)3, making the surfaces hydrophilic or hydrophobic. By the MD simulations of 6T, it was found that three stable azimuthal directions exist (0, ˜45, and 90° the angle that the c-axis makes with the groove), being consistent with experimental results. MD simulations of deposition processes of 6T and pentacene were also carried out, and pentacene molecules showed the spontaneous formation of herringbone packing during deposition. Some pentacene molecules stood on the surface and formed a cluster whose a-axis was parallel to the groove. It is expected that a deep understanding of the molecular-scale mechanisms will lead graphoepitaxy to practical applications, improving the performance of organic devices.

Growth of pentacene on α -Al2O3 (0001) studied by in situ optical spectroscopy

NASA Astrophysics Data System (ADS)

Zhang, Lei; Fu, X.; Hohage, M.; Zeppenfeld, P.; Sun, L. D.

2017-09-01

The growth of pentacene thin films on a sapphire α -Al2O3 (0001) surface was investigated in situ using differential reflectance spectroscopy (DRS). Two different film structures are observed depending on the substrate temperature. If pentacene is deposited at room temperature, a wetting layer consisting of flat-lying molecules is formed after which upright-standing molecular layers with a herringbone structure start to grow. At low substrate temperature of 100 K, the long molecular axis of the pentacene molecules remains parallel to the surface plane throughout the entire growth regime up to rather large thicknesses. Heating thin films deposited at 100 K to room temperature causes the pentacene molecules beyond the wetting layer to stand up and assemble into a herringbone structure. Another interesting observation is the dewetting of the first flat-lying monolayer upon exposure to air, leading to the condensation of islands consisting of upright-standing molecules. Our results emphasize the interplay between growth kinetics and thermodynamics and its influence on the molecular orientation in organic thin films.

Impact of molecular packing on electronic polarization in organic crystals: the case of pentacene vs TIPS-pentacene.

PubMed

Ryno, Sean M; Risko, Chad; Brédas, Jean-Luc

2014-04-30

Polarization energy corresponds to the stabilization of the cation or anion state of an atom or molecule when going from the gas phase to the solid state. The decrease in ionization energy and increase in electron affinity in the solid state are related to the (electronic and nuclear) polarization of the surrounding atoms and molecules in the presence of a charged entity. Here, through a combination of molecular mechanics and quantum mechanics calculations, we evaluate the polarization energies in two prototypical organic semiconductors, pentacene and 6,13-bis(2-(tri-isopropylsilyl)ethynyl)pentacene (TIPS-pentacene). Comparison of the results for the two systems reveals the critical role played by the molecular packing configurations in the determination of the polarization energies and provides physical insight into the experimental data reported by Lichtenberger and co-workers (J. Amer. Chem. Soc. 2010, 132, 580; J. Phys. Chem. C 2010, 114, 13838). Our results underline that the impact of packing configurations, well established in the case of the charge-transport properties, also extends to the polarization properties of π-conjugated materials.

Time Resolved Microscopy of Charge Trapping in Polycrystalline Pentacene

NASA Astrophysics Data System (ADS)

Jaquith, Michael; Muller, Erik; Marohn, John

2007-03-01

The microscopic mechanisms by which charges trap in organic electronic materials are poorly understood. Muller and Marohn recently showed that electric force microscopy (EFM) can be used to image trapped charge in working pentacene thin-film transistors [E. M. Muller et al., Adv. Mater. 17 1410 (2005)]. We have made a new discovery by imaging trapped charge in pentacene films with much larger grains. In contrast to the previous study in which charge was found to trap inhomogeneously throughout the transistor gap, we find microscopic evidence for a new trapping mechanism in which charges trap predominantly at the pentacene/metal interface in large-grained devices. We conclude that at least two charge trapping mechanisms are at play in polycrystalline pentacene. We have made localized measurements of the trap growth over time by performing pulsed-gate EFM experiments. Trap formation is not instantaneous, taking up to a second to complete. Furthermore, the charge-trapping rate depends strongly on gate voltage (or hole concentration). This kinetics data is consistent with the hypothesis that traps form by chemical reaction.

Angular-dependent EDMR linewidth for spin-dependent space charge limited conduction in a polycrystalline pentacene

NASA Astrophysics Data System (ADS)

Fukuda, Kunito; Asakawa, Naoki

2017-08-01

Spin-dependent space charge limited carrier conduction in a Schottky barrier diode using polycrystalline p-type π-conjugated molecular pentacene is explored using multiple-frequency electrically detected magnetic resonance (EDMR) spectroscopy with a variable-angle configuration. The measured EDMR spectra are decomposed into two components derived respectively from mobile and trapped positive polarons. The linewidth of the EDMR signal for the trapped polarons increases with increasing resonance magnetic field for an in-plane configuration where the normal vector of the device substrate is perpendicular to the resonance magnetic field, while it is independent of the field for an out-of-plane configuration. This difference is consistent with the pentacene arrangement on the device substrate, where pentacene molecules exhibit a uniaxial orientation on the out-of-substrate plane. By contrast, the mobile polarons do not show anisotropic behavior with respect to the resonance magnetic field, indicating that the anisotropic effect is averaged out owing to carrier motion. These results suggest that the orientational arrangements of polycrystalline pentacene molecules in a nano thin film play a crucial role in spin-dependent electrical conduction.

Crystallinity of the epitaxial heterojunction of C60 on single crystal pentacene

NASA Astrophysics Data System (ADS)

Tsuruta, Ryohei; Mizuno, Yuta; Hosokai, Takuya; Koganezawa, Tomoyuki; Ishii, Hisao; Nakayama, Yasuo

2017-06-01

The structure of pn heterojunctions is an important subject in the field of organic semiconductor devices. In this work, the crystallinity of an epitaxial pn heterojunction of C60 on single crystal pentacene is investigated by non-contact mode atomic force microscopy and high-resolution grazing incidence x-ray diffraction. Analysis shows that the C60 molecules assemble into grains consisting of single crystallites on the pentacene single crystal surface. The in-plane mean crystallite size exceeds 0.1 μm, which is at least five time larger than the size of crystallites deposited onto polycrystalline pentacene thin films grown on SiO2. The results indicate that improvement in the crystal quality of the underlying molecular substrate leads to drastic promotion of the crystallinity at the organic semiconductor heterojunction.

Molecular charge distribution and dispersion of electronic states in the contact layer between pentacene and Cu(119) and beyond

NASA Astrophysics Data System (ADS)

Annese, E.; Fujii, J.; Baldacchini, C.; Zhou, B.; Viol, C. E.; Vobornik, I.; Betti, M. G.; Rossi, G.

2008-05-01

The interaction of pentacene molecules in contact with the Cu(119) stepped surface has been directly imaged by scanning tunneling microscopy and analyzed by angle resolved photoemission spectroscopy. Interacting molecules, which are in contact with copper, generate dispersive electronic states associated with a perturbed electron charge density distribution of the molecular orbitals. In contrast, the electron charge density of molecules of the pentacene on top of the first layer, which is not in direct contact with the Cu surface, shows an intramolecular structure very similar to that of the free molecule. Our results indicate that the delocalization of the molecular states in the pentacene/Cu system is confined to the very first molecular layer at the interface.

Identification of an organic semiconductor superlattice structure of pentacene and perfluoro-pentacene through resonant and non-resonant X-ray scattering

DOE PAGES

Kowarik, S.; Hinderhofer, A.; Wang, C.; ...

2015-11-30

Highly crystalline and stable molecular superlattices are grown with the smallest possible stacking period using monolayers (MLs) of the organic semiconductors pentacene (PEN) and perfluoro-pentacene (PFP). Superlattice reflections in X-ray reflectivity and their energy dependence in resonant soft X-ray reflectivity measurements show that PFP and PEN MLs indeed alternate even though the coherent ordering is lost after ~ 4 ML. The observed lattice spacing of 15.9 Å in the superlattice is larger than in pure PEN and PFP films, presumably because of more upright standing molecules and lack of interdigitation between the incommensurate crystalline PEN and PFP layers. The findingsmore » are important for the development of novel organic quantum optoelectronic devices.« less

Novel surface diffusion characteristics for a robust pentacene derivative on Au(1 1 1) surfaces

NASA Astrophysics Data System (ADS)

Miller, Ryan A.; Larson, Amanda; Pohl, Karsten

2017-06-01

Molecular dynamics simulations have been performed in both the ab initio and classical mechanics frameworks of 5,6,7-trithiapentacene-13-one (TTPO) molecules on flat Au(1 1 1) surfaces. Results show new surface diffusion characteristics including a strong preference for the molecule to align its long axis parallel to the sixfold Au(1 1 1) symmetry directions and subsequently diffuse along these close-packed directions, and a calculated activation energy for diffusion of 0.142 eV, about four times larger than that for pure pentacene on Au. The temperature-dependent diffusion coefficients were calculated to help quantify the molecular mobility during the experimentally observed process of forming self-assembled monolayers on gold electrodes.

High-mobility, aligned crystalline domains of TIPS-pentacene with metastable polymorphs through lateral confinement of crystal growth.

PubMed

Giri, Gaurav; Park, Steve; Vosgueritchian, Michael; Shulaker, Max Marcel; Bao, Zhenan

2014-01-22

Patterns composed of solvent wetting and dewetting regions promote lateral confinement of solution-sheared and lattice-strained TIPS-pentacene crystals. This lateral confinement causes aligned crystal growth, and the smallest patterns of 0.5 μm wide solvent wetting regions promotes formation of highly strained, aligned, and single-crystalline TIPS-pentacene regions with mobility as high as 2.7 cm(2) V(-1) s(-1) . © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Excited-state dynamics of pentacene derivatives with stable radical substituents.

PubMed

Ito, Akitaka; Shimizu, Akihiro; Kishida, Noriaki; Kawanaka, Yusuke; Kosumi, Daisuke; Hashimoto, Hideki; Teki, Yoshio

2014-06-23

The excited-state dynamics of pentacene derivatives with stable radical substituents were evaluated in detail through transient absorption measurements. The derivatives showed ultrafast formation of triplet excited state(s) in the pentacene moiety from a photoexcited singlet state through the contributions of enhanced intersystem crossing and singlet fission. Detailed kinetic analyses for the transient absorption data were conducted to quantify the excited-state characteristics of the derivatives. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Optical Spectra and Kinetics of Single Impurity Molecules in a Polymer: Spectral Diffusion and Persistent Spectral Hole-Burning

DTIC Science & Technology

1991-11-07

new area of opticAl sp,,ctroscopy of solids where truly unique single environments and quantum effects can be studied in detail. In the pentacene in p...observed. Until very recentlx, the reports of SMI) have concentrated on the crystalline system of pentacene in p-terphenyl. Owing to the complex physical...excessive PSIIB, pentacene in benzoi, acid, is described briefly. The advantages of the perylene in PF_. system become evident immediately when

Why bistetracenes are much less reactive than pentacenes in Diels-Alder reactions with fullerenes.

PubMed

Cao, Yang; Liang, Yong; Zhang, Lei; Osuna, Sílvia; Hoyt, Andra-Lisa M; Briseno, Alejandro L; Houk, K N

2014-07-30

The Diels-Alder (DA) reactions of pentacene (PT), 6,13-bis(2-trimethylsilylethynyl)pentacene (TMS-PT), bistetracene (BT), and 8,17-bis(2-trimethylsilylethynyl)bistetracene (TMS-BT) with the [6,6] double bond of [60]fullerene have been investigated by density functional theory calculations. Reaction barriers and free energies have been obtained to assess the effects of frameworks and substituent groups on the DA reactivity and product stability. Calculations indicate that TMS-BT is about 5 orders of magnitude less reactive than TMS-PT in the reactions with [60]fullerene. This accounts for the observed much higher stability of TIPS-BT than TIPS-PT when mixed with PCBM. Surprisingly, calculations predict that the bulky silylethynyl substituents of TMS-PT and TMS-BT have only a small influence on reaction barriers. However, the silylethynyl substituents significantly destabilize the corresponding products due to steric repulsions in the adducts. This is confirmed by experimental results here. Architectures of the polycyclic aromatic hydrocarbons (PAHs) play a crucial role in determining both the DA barrier and the adduct stability. The reactivities of different sites in various PAHs are related to the loss of aromaticity, which can be predicted using the simple Hückel molecular orbital localization energy calculations.

Ultrafast carrier dynamics in organic molecular crystals and conjugated polymers

NASA Astrophysics Data System (ADS)

Hegmann, Frank

2005-03-01

Organic semiconductors are being extensively studied by many research groups around the world for applications in electronic and photonic devices. For example, much work has focused on the development of organic thin film transistors based on thermally evaporated pentacene films, where the polycrystalline morphology typically results in a thermally-activated carrier mobility. On the other hand, more intrinsic bandlike transport, where the carrier mobility increases as the temperature decreases, has been observed in many organic single crystals. However, the nature of charge transport in organic molecular crystals is still not understood. Also, despite many advances in organic photonics, the nature of photocarrier generation in organic semiconductors is not completely understood and remains controversial even today. The generation of mobile charge carriers in photoexcited organic materials occurs over femtosecond to picosecond time scales, and so ultrafast pump-probe experiments are essential in order to improve our understanding of fundamental processes in these materials. Recently, time-resolved terahertz pulse spectroscopy has been used to directly probe transient photoconductivity in pentacene and functionalized pentacene thin films and single crystals [1,2], revealing photogeneration of mobile charge carriers over sub-picosecond time scales as well as bandlike carrier transport in both single crystal and thin film samples [1]. This talk will provide an overview of ultrafast carrier dynamics in organic semiconductors, and will emphasize how time-resolved terahertz pulse spectroscopy can be used to help understand the nature of photoexcitations and carrier transport in organic materials. (This work was supported by NSERC, CFI, CIPI, the Killam Trust, and ONR. Collaborators for this work are listed in Ref. 1.) [1] O. Ostroverkhova, D. G. Cooke, S. Shcherbyna, R. F. Egerton, F. A. Hegmann, R. R. Tykwinski, and J. E. Anthony, Phys. Rev. B., in press. [2] V. K. Thorsmølle, R. D. Averitt, X. Chi, D. J. Hilton, D. L. Smith, A. P. Ramirez, and A. J. Taylor, Appl. Phys. Lett. 84, 891 (2004).

Low-voltage high-performance organic thin film transistors with a thermally annealed polystyrene/hafnium oxide dielectric

NASA Astrophysics Data System (ADS)

Wang, Ying; Acton, Orb; Ting, Guy; Weidner, Tobias; Ma, Hong; Castner, David G.; Jen, Alex K.-Y.

2009-12-01

Low-voltage pentacene-based organic thin film transistors (OTFTs) are demonstrated with polystyrene (PS)/hafnium oxide (HfOx) hybrid dielectrics. Thermal annealing of PS films on HfOx at 120 °C (PS-120) induces a flatter orientation of the phenyl groups (tilt angle 65°) at the surface compared to PS films without annealing (PS-RT) (tilt angle 31°). The flatter phenyl group orientation leads to better matching of surface energy between pentacene and PS. Pentacene deposited on PS-120 display higher quality thin films with larger grain sizes and higher crystallinity. Pentacene OTFTs with PS-120/HfOx hybrid dielectrics can operate at low-voltage (<3 V) with high field-effect mobilities (1 cm2/V s), high on/off current ratios (106), and low subthreshold slopes (100 mV/dec).

Epitaxially Grown Films of Standing and Lying Pentacene Molecules on Cu(110) Surfaces

PubMed Central

2011-01-01

Here, it is shown that pentacene thin films (30 nm) with distinctively different crystallographic structures and molecular orientations can be grown under essentially identical growth conditions in UHV on clean Cu(110) surfaces. By X-ray diffraction, we show that the epitaxially oriented pentacene films crystallize either in the “thin film” phase with standing molecules or in the “single crystal” structure with molecules lying with their long axes parallel to the substrate. The morphology of the samples observed by atomic force microscopy shows an epitaxial alignment of pentacene crystallites, which corroborates the molecular orientation observed by X-ray diffraction pole figures. Low energy electron diffraction measurements reveal that these dissimilar growth behaviors are induced by subtle differences in the monolayer structures formed by slightly different preparation procedures. PMID:21479111

"Doping" pentacene with sp(2)-phosphorus atoms: towards high performance ambipolar semiconductors.

PubMed

Long, Guankui; Yang, Xuan; Chen, Wangqiao; Zhang, Mingtao; Zhao, Yang; Chen, Yongsheng; Zhang, Qichun

2016-01-28

Recent research progress in black phosphorus sheets strongly encourages us to employ pentacene as a parent system to systematically investigate how the "doping" of sp(2)-phosphorus atoms onto the backbone of pentacene influences its optical and charge transport properties. Our theoretical investigations proved that increasing the contribution of the pz atomic orbital of the sp(2)-phosphorus to the frontier molecular orbital of phosphapentacenes could significantly decrease both hole and electron reorganization energies and dramatically red-shift the absorption of pentacene. The record smallest hole and electron reorganization energies of 69.80 and 95.74 meV for heteropentacene derivatives were obtained. These results suggest that phosphapentacenes (or phosphaacenes) could be potential promising candidates to achieve both higher and balanced mobilities in organic field effect transistors and realize a better power conversion efficiency in organic photovoltaics.

Excitons in molecular crystals from first-principles many-body perturbation theory: Picene versus pentacene

NASA Astrophysics Data System (ADS)

Cudazzo, Pierluigi; Gatti, Matteo; Rubio, Angel

2012-11-01

By solving the first-principles many-body Bethe-Salpeter equation, we compare the optical properties of two prototype and technological relevant organic molecular crystals: picene and pentacene. Albeit very similar for the structural and electronic properties, picene and pentacene show remarkable differences in their optical spectra. While for pentacene the absorption onset is due to a charge-transfer exciton, in picene it is related to a strongly localized Frenkel exciton. The detailed comparison between the two materials allows us to discuss, on general grounds, how the interplay between the electronic band dispersion and the exchange electron-hole interaction plays a fundamental role in setting the nature of the exciton. It represents a clear example of the relevance of the competition between localization and delocalization in the description of two-particle electronic correlation.

A low-frequency noise model with carrier generation-recombination process for pentacene organic thin-film transistor

NASA Astrophysics Data System (ADS)

Han, C. Y.; Qian, L. X.; Leung, C. H.; Che, C. M.; Lai, P. T.

2013-07-01

By including the generation-recombination process of charge carriers in conduction channel, a model for low-frequency noise in pentacene organic thin-film transistors (OTFTs) is proposed. In this model, the slope and magnitude of power spectral density for low-frequency noise are related to the traps in the gate dielectric and accumulation layer of the OTFT for the first time. The model can well fit the measured low-frequency noise data of pentacene OTFTs with HfO2 or HfLaO gate dielectric, which validates this model, thus providing an estimate on the densities of traps in the gate dielectric and accumulation layer. It is revealed that the traps in the accumulation layer are much more than those in the gate dielectric, and so dominate the low-frequency noise of pentacene OTFTs.

Theoretical comparative studies on transport properties of pentacene, pentathienoacene, and 6,13-dichloropentacene.

PubMed

Zhang, Xu; Yang, Xiaodi; Geng, Hua; Nan, Guangjun; Sun, Xingwen; Xi, Jinyang; Xu, Xin

2015-05-05

Pentacene derivative 6,13-dichloropentacene (DCP) is one of the latest additions to the family of organic semiconductors with a great potential for use in transistors. We carry out a detailed theoretical calculation for DCP, with systematical comparison to pentacene, pentathienoacene (PTA, the thiophene equivalent of pentacene), to gain insights in the theoretical design of organic transport materials. The charge transport parameters and carrier mobilities are investigated from the first-principles calculations, based on the widely used Marcus electron transfer theory and quantum nuclear tunneling model, coupled with random walk simulation. Molecular structure and the crystal packing type are essential to understand the differences in their transport behaviors. With the effect of molecule modification, significant one-dimensional π-stacks are found within the molecular layer in PTA and DCP crystals. The charge transport along the a-axis plays a dominant role for the carrier mobilities in the DCP crystal due to the strong transfer integrals within the a-axis. Pentacene shows a relatively large 3D mobility. This is attributed to the relatively uniform electronic couplings, which thus provides more transport pathways. PTA has a much smaller 3D mobility than pentacene and DCP for the obvious increase of the reorganization energy with the introduction of thiophene. It is found that PTA and DCP exhibit lower HOMO (highest occupied molecular orbital) levels and better environmental stability, indicating the potential applications in organic electronics. © 2015 Wiley Periodicals, Inc.

Electron transfer beyond the static picture: A TDDFT/TD-ZINDO study of a pentacene dimer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reslan, Randa; Lopata, Kenneth; Arntsen, Christopher

2012-12-14

We use time-dependent density functional theory and time-dependent ZINDO (a semi-empirical method) to study transfer of an extra electron between a pair of pentacene molecules. A measure of the electronic transfer integral is computed in a dynamic picture via the vertical excitation energy from a delocalized anionic ground state. With increasing dimer separation, this dynamical measurement of charge transfer is shown to be significantly larger than the commonly used static approximation (i.e., LUMO+1–LUMO of the neutral dimer, or HOMO–LUMO of the charged dimer), up to an order of magnitude higher at 6 Å. These results offer a word of cautionmore » for calculations involving large separations, as in organic photovoltaics, where care must be taken when using a static picture to model charge transfer.« less

Electron transfer beyond the static picture: A TDDFT/TD-ZINDO study of a pentacene dimer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reslan, Randa; Lopata, Kenneth A.; Arntsen, Christopher D.

2012-12-14

We use time-dependent density functional theory and time-dependent ZINDO (a semi-empirical method) to study transfer of an extra electron between a pair of pentacene dimers. A measure of the electronic transfer integral is computed in a dynamic picture via the vertical excitation energy from a delocalized anionic ground state. With increasing dimer separation, this dynamical measurement of charge transfer is shown to be significantly larger than the commonly used static approximation (i.e., LUMO+1 - LUMO of the neutral dimer, or HOMO - LUMO of the charged dimer), up to an order of magnitude higher at 6 Å. These results offermore » a word of caution for calculations involving large separations, as in organic photovoltaics, where care must be taken when using a static picture to model charge transfer.« less

Pentacene Excitons in Strong Electric Fields.

PubMed

Kuhnke, Klaus; Turkowski, Volodymyr; Kabakchiev, Alexander; Lutz, Theresa; Rahman, Talat S; Kern, Klaus

2018-02-05

Electroluminescence spectroscopy of organic semiconductors in the junction of a scanning tunneling microscope (STM) provides access to the polarizability of neutral excited states in a well-characterized molecular geometry. We study the Stark shift of the self-trapped lowest singlet exciton at 1.6 eV in a pentacene nanocrystal. Combination of density functional theory (DFT) and time-dependent DFT (TDDFT) with experiment allows for assignment of the observation to a charge-transfer (CT) exciton. Its charge separation is perpendicular to the applied field, as the measured polarizability is moderate and the electric field in the STM junction is strong enough to dissociate a CT exciton polarized parallel to the applied field. The calculated electric-field-induced anisotropy of the exciton potential energy surface will also be of relevance to photovoltaic applications. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Surface properties of SiO2 with and without H2O2 treatment as gate dielectrics for pentacene thin-film transistor applications

NASA Astrophysics Data System (ADS)

Hung, Cheng-Chun; Lin, Yow-Jon

2018-01-01

The effect of H2O2 treatment on the surface properties of SiO2 is studied. H2O2 treatment leads to the formation of Si(sbnd OH)x at the SiO2 surface that serves to reduce the number of trap states, inducing the shift of the Fermi level toward the conduction band minimum. H2O2 treatment also leads to a noticeable reduction in the value of the SiO2 capacitance per unit area. The effect of SiO2 layers with H2O2 treatment on the behavior of carrier transports for the pentacene/SiO2-based organic thin-film transistor (OTFT) is also studied. Experimental identification confirms that the shift of the threshold voltage towards negative gate-source voltages is due to the reduced number of trap states in SiO2 near the pentacene/SiO2 interface. The existence of a hydrogenated layer between pentacene and SiO2 leads to a change in the pentacene-SiO2 interaction, increasing the value of the carrier mobility.

Tautomerization and Dimerization of 6,13-Disubstituted Derivatives of Pentacene.

PubMed

Garcia-Borràs, Marc; Konishi, Akihito; Waterloo, Andreas; Liang, Yong; Cao, Yang; Hetzer, Constantin; Lehnherr, Dan; Hampel, Frank; Houk, Kendall N; Tykwinski, Rik R

2017-05-02

Two new 6,13-disubstituted pentacene derivatives, 1 c and 1 d, with alkyl and triisopropylsilylethynyl substitution have been synthesized and characterized experimentally and computationally. The alkyl substituted 1 c and 1 d represent the first 6-alkyl-substituted pentacene derivative where the fully aromatic species dominates over the corresponding tautomer. Indeed, no tautomerization product is found for either 1 c or 1 d upon heating or in the presence of catalytic amounts of acid. On the other hand, an unexpected dimer (3 c) is formed from 1 c. A plausible mechanism for this new dimerization process of the 6-methyl-substituted pentacene derivative 1 c is proposed, which involves first a bimolecular hydrogen atom transfer followed by an intramolecular [4+2] Diels-Alder cycloaddition. In the case of 6-butyl substitution, neither tautomerization nor dimerization is observed. Computations support the proposed 1 c dehydrodimerization pathway, explain why 1 d does not dimerize, and show the importance of the nature of the group at C-13 in controlling the relative stability of 6-alkyl-substituted pentacene tautomers. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Structural fluctuation governed dynamic diradical character in pentacene.

PubMed

Yang, Hongfang; Chen, Mengzhen; Song, Xinyu; Bu, Yuxiang

2015-06-07

We unravel intriguing dynamical diradical behavior governed by structural fluctuation in pentacene using ab initio molecular dynamics simulation. In contrast to static equilibrium configuration of pentacene with a closed-shell ground state without diradical character, due to structural fluctuation, some of its dynamical snapshot configurations exhibit an open-shell broken-symmetry singlet ground state with diradical character, and such diradical character presents irregular pulsing behavior in time evolution. Not all structural changes can lead to diradical character, only those involving the shortening of cross-linking C-C bonds and variations of the C-C bonds in polyacetylene chains are the main contributors. This scenario about diradicalization is distinctly different from that in long acenes. The essence is that structural distortion cooperatively raises the HOMO and lowers the LUMO, efficiently reducing the HOMO-LUMO and singlet-triplet energy gaps, which facilitate the formation of a broken-symmetry open-shell singlet state. The irregular pulsing behavior originates from the mixing of normal vibrations in pentacene. This fascinating behavior suggests the potential application of pentacene as a suitable building block in the design of new electronic devices due to its magnetism-controllability through energy induction. This work provides new insight into inherent electronic property fluctuation in acenes.

Technology development of high-quality semiconductor devices using solution-processed crystallization of pentacene

NASA Astrophysics Data System (ADS)

Liu, Hung-Wei

Organic electronic materials and processing techniques have attracted considerable attention for developing organic thin-film transistors (OTFTs), since they may be patterned on flexible substrates which may be bent into a variety of shapes for applications such as displays, smart cards, solar devices and sensors Various fabrication methods for building pentacene-based OTFTs have been demonstrated. Traditional vacuum deposition and vapor deposition methods have been studied for deposition on plastic and paper, but these are unlikely to scale well to large area printing. Researchers have developed methods for processing OTFTs from solution because of the potential for low-cost and large area device manufacturing, such as through inkjet or offset printing. Most methods require the use of precursors which are used to make pentacene soluble, and these methods have typically produced much lower carrier mobility than the best vacuum deposited devices. We have investigated devices built from solution-processed pentacene that is locally crystallized at room temperature on the polymer substrates. Pentacene crystals grown in this manner are highly localized at pre-determined sites, have good crystallinity and show good carrier mobility, making this an attractive method for large area manufacturing of semiconductor devices.

Morphology and electronic transport of polycrystalline pentacene thin-film transistors

NASA Astrophysics Data System (ADS)

Knipp, D.; Street, R. A.; Völkel, A. R.

2003-06-01

Temperature-dependent measurements of thin-film transistors were performed to gain insight in the electronic transport of polycrystalline pentacene. Devices were fabricated with plasma-enhanced chemical vapor deposited silicon nitride gate dielectrics. The influence of the dielectric roughness and the deposition temperature of the thermally evaporated pentacene films were studied. Although films on rougher gate dielectrics and films prepared at low deposition temperatures exhibit similar grain size, the electronic properties are different. Increasing the dielectric roughness reduces the free carrier mobility, while low substrate temperature leads to more and deeper hole traps.

Coupling between Transport and Injection Properties of Pentacene Field-Effect Transistors with Different Morphologies

NASA Astrophysics Data System (ADS)

Lee, Keanchuan; Weis, Martin; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2013-08-01

We investigated the injection and transport properties of pentacene organic field-effect transistors (OFETs) with inclined and lamellar pentacene grains at various mutual ratios. Although the threshold voltage was conserved and no additional trapping on grain boundaries was suggested from the current-voltage measurements, the contact resistance and mobility increased linearly with the lamellar phase content. We showed that a model based on the coupling between both transport and injection properties via a space charge field caused by injected and trapped carriers accounts for these results.

Terahertz study of hole transport in pentacene thin films

NASA Astrophysics Data System (ADS)

Engelbrecht, Stefan G.; Prinz, Markus; Arend, Thomas R.; Kersting, Roland

2014-10-01

Terahertz electromodulation spectroscopy is a novel tool for studying charge carrier transport in polycrys­talline thin films. The technique selectively probes the high-frequency response of mobile carriers and is insensitive to scattering at grain boundaries as well as to trapping processes. In thin films of pentacene we find a hole mobility of 21 cm2 /Vs, which exceeds the largest previously reported values obtained in poly­ crystalline pentacene. Additionally, the data provide an upper limit of the hole conductivity effective mass of mh ≍ 0.8 me.

Self-interaction corrections applied to Mg-porphyrin, C60, and pentacene molecules

NASA Astrophysics Data System (ADS)

Pederson, Mark R.; Baruah, Tunna; Kao, Der-you; Basurto, Luis

2016-04-01

We have applied a recently developed method to incorporate the self-interaction correction through Fermi orbitals to Mg-porphyrin, C60, and pentacene molecules. The Fermi-Löwdin orbitals are localized and unitarily invariant to the Kohn-Sham orbitals from which they are constructed. The self-interaction-corrected energy is obtained variationally leading to an optimum set of Fermi-Löwdin orbitals (orthonormalized Fermi orbitals) that gives the minimum energy. A Fermi orbital, by definition, is dependent on a certain point which is referred to as the descriptor position. The degree to which the initial choice of descriptor positions influences the variational approach to the minimum and the complexity of the energy landscape as a function of Fermi-orbital descriptors is examined in detail for Mg-porphyrin. The applications presented here also demonstrate that the method can be applied to larger molecular systems containing a few hundred electrons. The atomization energy of the C60 molecule within the Fermi-Löwdin-orbital self-interaction-correction approach is significantly improved compared to local density approximation in the Perdew-Wang 92 functional and generalized gradient approximation of Perdew-Burke-Ernzerhof functionals. The eigenvalues of the highest occupied molecular orbitals show qualitative improvement.

Growth of long triisopropylsilylethynyl pentacene (TIPS-PEN) nanofibrils in a polymer thin film during spin-coating.

PubMed

Park, Minwoo; Min, Yuho; Lee, Yu-Jeong; Jeong, Unyong

2014-03-01

This study demonstrates the growth of long triisopropylsilyethynyl pentacene (TIPS-PEN) nanofibrils in a thin film of a crystalline polymer, poly(ε-caprolactone) (PCL). During spin-coating, TIPS-PEN molecules are locally extracted around the PCL grain boundaries and they crystallize into [010] direction forming long nanofibrils. Molecular weight of PCL and weight fraction (α) of TIPS-PEN in PCL matrix are key factors to the growth of nanofibrils. Long high-quality TIPS-PEN nanofibrils are obtained with high-molecular-weight PCL and at the α values in the range of 0.03-0.1. The long nanofibrils are used as an active layer in a field-effect organic transistor. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Flexible AMOLED backplane using pentacene TFT

NASA Astrophysics Data System (ADS)

Song, Chung Kun; Ryu, Gi Seong

2005-01-01

In this paper we fabricated a panel consisting of an array of organic TFTs (OTFT) and organic LEDs (OLED) in order to demonstrate the possible application of OTFTs to flexible active matrix OLED (AMOLED). The panel was composed of 64×64 pixels on 4 inch size PET substrate in which each pixel had one OTFT integrated with one green OLED. The panel successfully demonstrated to display some letters and pictures by emitting green light with luminance of 20 cd/m2 at 6 V, which was controlled by the gate voltage of OTFT. In addition we also developed fabrication processes for pentacene TFT with PVP gate on PET substrate. The OTFTs produced the maximum mobility of 1.2 cm2/V"sec and on/off current ratio of 2×106.

Scanning Tunneling Microscopy Analysis of a Pentacene/Graphene/SiC(0001) system

NASA Astrophysics Data System (ADS)

Yost, Andrew; Suzer, Ozgun; Smerdon, Joseph; Chien, Teyu; Guest, Jeffrey

2014-03-01

A complete understanding of the structure of molecular assemblies, as well as an understanding of donor-acceptor interactions is crucial in the development of emergent molecular electronics technologies such as organic photovoltaics. The pentacene (C22H14) is a good electron donor in Pentacene-C60 system, which is a model system of an organic photovoltaic cell.. Here we present scanning tunneling microscopy studies of the pentacene(Pn) molecule on Graphene(G) that is epitaxially grown on SiC(0001). In addition to the morphologies reported in literature, several new structures of Pn on on G/SiC(0001) were observed with different periodicity and registry both in monolayer and bilayer coverages of molecules on the surface. Preliminary scanning tunneling spectroscopy of the molecular system is also discussed; well-isolated states and a large HOMO-LUMO gap indicate the Pn is weakly coupled to the grapheme and underlying substrate.

Trap-mediated electronic transport properties of gate-tunable pentacene/MoS2 p-n heterojunction diodes

PubMed Central

Kim, Jae-Keun; Cho, Kyungjune; Kim, Tae-Young; Pak, Jinsu; Jang, Jingon; Song, Younggul; Kim, Youngrok; Choi, Barbara Yuri; Chung, Seungjun; Hong, Woong-Ki; Lee, Takhee

2016-01-01

We investigated the trap-mediated electronic transport properties of pentacene/molybdenum disulphide (MoS2) p-n heterojunction devices. We observed that the hybrid p-n heterojunctions were gate-tunable and were strongly affected by trap-assisted tunnelling through the van der Waals gap at the heterojunction interfaces between MoS2 and pentacene. The pentacene/MoS2 p-n heterojunction diodes had gate-tunable high ideality factor, which resulted from trap-mediated conduction nature of devices. From the temperature-variable current-voltage measurement, a space-charge-limited conduction and a variable range hopping conduction at a low temperature were suggested as the gate-tunable charge transport characteristics of these hybrid p-n heterojunctions. Our study provides a better understanding of the trap-mediated electronic transport properties in organic/2-dimensional material hybrid heterojunction devices. PMID:27829663

Tandem organic light-emitting diodes with buffer-modified C60/pentacene as charge generation layer

NASA Astrophysics Data System (ADS)

Wang, Zhen; Zheng, Xin; Liu, Fei; Wang, Pei; Gan, Lin; Wang, Jing-jing

2017-09-01

Buffer-modified C60/pentacene as charge generation layer (CGL) is investigated to achieve effective performance of charge generation. Undoped green electroluminescent tandem organic light-emitting diodes (OLEDs) with multiple identical emissive units and using buffer-modified C60/pentacene organic semiconductor heterojunction (OHJ) as CGL are demonstrated to exhibit better current density and brightness, compared with conventional single-unit devices. The current density and brightness both can be significantly improved with increasing the thickness of Al. However, excessive thickness of Al seriously decreases the transmittance of films and damages the interface. As a result, the maximum current efficiency of 1.43 cd·A-1 at 30 mA·cm-2 can be achieved for tandem OLEDs with optimal thickness of Al. These results clearly demonstrate that Cs2CO3/Al is an effective buffer for C60/pentacene-based tandem OLEDs.

Robust singlet fission in pentacene thin films with tuned charge transfer interactions.

PubMed

Broch, K; Dieterle, J; Branchi, F; Hestand, N J; Olivier, Y; Tamura, H; Cruz, C; Nichols, V M; Hinderhofer, A; Beljonne, D; Spano, F C; Cerullo, G; Bardeen, C J; Schreiber, F

2018-03-05

Singlet fission, the spin-allowed photophysical process converting an excited singlet state into two triplet states, has attracted significant attention for device applications. Research so far has focused mainly on the understanding of singlet fission in pure materials, yet blends offer the promise of a controlled tuning of intermolecular interactions, impacting singlet fission efficiencies. Here we report a study of singlet fission in mixtures of pentacene with weakly interacting spacer molecules. Comparison of experimentally determined stationary optical properties and theoretical calculations indicates a reduction of charge-transfer interactions between pentacene molecules with increasing spacer molecule fraction. Theory predicts that the reduced interactions slow down singlet fission in these blends, but surprisingly we find that singlet fission occurs on a timescale comparable to that in pure crystalline pentacene. We explain the observed robustness of singlet fission in such mixed films by a mechanism of exciton diffusion to hot spots with closer intermolecular spacings.

Clean Transfer of Wafer-Scale Graphene via Liquid Phase Removal of Polycyclic Aromatic Hydrocarbons.

PubMed

Kim, Hyun Ho; Kang, Boseok; Suk, Ji Won; Li, Nannan; Kim, Kwang S; Ruoff, Rodney S; Lee, Wi Hyoung; Cho, Kilwon

2015-05-26

Pentacene (C22H14), a polycyclic aromatic hydrocarbon, was used as both supporting and sacrificing layers for the clean and doping-free graphene transfer. After successful transfer of graphene to a target substrate, the pentacene layer was physically removed from the graphene surface by using intercalating organic solvent. This solvent-mediated removal of pentacene from graphene surface was investigated by both theoretical calculation and experimental studies with various solvents. The uses of pentacene and appropriate intercalation solvent enabled graphene transfer without forming a residue from the supporting layer. Such residues tend to cause charged impurity scattering and unintentional graphene doping effects. As a result, this clean graphene exhibited extremely homogeneous surface potential profiles over a large area. A field-effect transistor fabricated using this graphene displayed a high hole (electron) mobility of 8050 cm(2)/V·s (9940 cm(2)/V·s) with a nearly zero Dirac point voltage.

Effect of co-crystallization on singlet fission efficiency in pentacene derivatives

NASA Astrophysics Data System (ADS)

Wang, Xiaopeng; Sanders, Samuel; Campos, Luis; Sfeir, Matthew; Marom, Noa

Singlet fission (SF), the conversion of one singlet exciton into two triplet excitons, may lead to a twofold increase in the efficiency of organic photovoltaics. Since SF has been observed in crystalline pentacene, this material has drawn interest both experimentally and theoretically. Recently, it has been shown that SF efficiency in rubrene may be improved by modifying the crystal packing. Here, we study the effect of co-crystallization with small molecule H-bond donors on SF efficiency in pentacene derivatives. Five co-crystals are synthetized and their photoluminescence (PL) and absorption spectra are measured. First-principles calculations based on many-body perturbation theory (MBPT) are then employed to study their excitonic properties. By combining experiment and theory, we demonsrate that excitonic properties, including singlet-triplet gaps, exciton binding energies, and exciton localization, are significantly modulated in pentacene co-crystals. Consequently, co-crystallization becomes an effective strategy for improving SF efficiency in molecular crystals of organic semiconductors.

Time-resolved electric force microscopy of charge traps in polycrystalline pentacene films

NASA Astrophysics Data System (ADS)

Jaquith, Michael; Muller, Erik; Marohn, John

2006-03-01

The microscopic mechanisms by which charges trap in organic electronic materials are poorly understood. Muller and Marohn recently showed that electric force microscopy (EFM) can be used to image trapped charge in working pentacene thin-film transistors [E. M. Muller et al, Adv. Mater. 17 1410 (2005)]. We have extended their work by imaging trapped charge in pentacene films with much larger grains. In contrast to the previous study in which charge was found to trap inhomogeneously throughout the transistor gap, we find microscopic evidence for a new trapping mechanism in which charges trap predominantly at the pentacene/metal interface in large-grained devices. We have also made localized measurements of the trap growth over time by performing pulsed-gate EFM experiments. Integrated-rate kinetics data supports a charge trap mechanism which is second order in holes, e.g., holes trap in pairs, although the charge-trapping rate appears to depend on gate voltage.

Molecular-scale properties of MoO3 -doped pentacene

NASA Astrophysics Data System (ADS)

Ha, Sieu D.; Meyer, Jens; Kahn, Antoine

2010-10-01

The mechanisms of molecular doping in organic electronic materials are explored through investigation of pentacene p -doped with molybdenum trioxide (MoO3) . Doping is confirmed with ultraviolet photoelectron spectroscopy. Isolated dopants are imaged at the molecular scale using scanning tunneling microscopy (STM) and effects due to localized holes are observed. The results demonstrate that donated charges are localized by the counterpotential of ionized dopants in MoO3 -doped pentacene, generalizing similar effects previously observed for pentacene doped with tetrafluoro-tetracyanoquinodimethane. Such localized hole effects are only observed for low molecular weight MoO3 species. It is shown that for larger MoO3 polymers and clusters, the ionized dopant potential is sufficiently large as to mask the effect of the localized hole in STM images. Current-voltage measurements recorded using scanning tunneling spectroscopy reveal that electron conductivity decreases in MoO3 -doped films, as expected for electron capture and p -doping.

Photocurrent measurements of pentacene-based devices

NASA Astrophysics Data System (ADS)

Masurkar, Amrita; Kymissis, Ioannis

2015-09-01

Photocurrent spectroscopy (PCS) and photocurrent microscopy (PCM) are powerful tools that can probe the underlying mechanisms of charge generation and transport in organic semiconductor devices. There has been significant progress in the use of these techniques, which has yielded a number of insights into the underlying materials and operation of the devices. Despite the potential for PCS and PCM to become standard tools, however, a consensus has not been reached on (1) its uses and (2) the underlying mechanisms which produce the photoresponse. This is particularly true for measurements of pentacene devices, as the energy dynamics of pentacene are complex. Accordingly, here we report the current body of PCS and PCM of pentacene devices, offer interpretations of the data, and discuss which questions remain unanswered. We have divided the reviewed work into four categories based on the goals of the study and the technique used: photocurrent spectroscopy, scanning photocurrent microscopy, mobility, and trap density-of-states.

Trap-mediated electronic transport properties of gate-tunable pentacene/MoS2 p-n heterojunction diodes

NASA Astrophysics Data System (ADS)

Kim, Jae-Keun; Cho, Kyungjune; Kim, Tae-Young; Pak, Jinsu; Jang, Jingon; Song, Younggul; Kim, Youngrok; Choi, Barbara Yuri; Chung, Seungjun; Hong, Woong-Ki; Lee, Takhee

2016-11-01

We investigated the trap-mediated electronic transport properties of pentacene/molybdenum disulphide (MoS2) p-n heterojunction devices. We observed that the hybrid p-n heterojunctions were gate-tunable and were strongly affected by trap-assisted tunnelling through the van der Waals gap at the heterojunction interfaces between MoS2 and pentacene. The pentacene/MoS2 p-n heterojunction diodes had gate-tunable high ideality factor, which resulted from trap-mediated conduction nature of devices. From the temperature-variable current-voltage measurement, a space-charge-limited conduction and a variable range hopping conduction at a low temperature were suggested as the gate-tunable charge transport characteristics of these hybrid p-n heterojunctions. Our study provides a better understanding of the trap-mediated electronic transport properties in organic/2-dimensional material hybrid heterojunction devices.

Trap-mediated electronic transport properties of gate-tunable pentacene/MoS2 p-n heterojunction diodes.

PubMed

Kim, Jae-Keun; Cho, Kyungjune; Kim, Tae-Young; Pak, Jinsu; Jang, Jingon; Song, Younggul; Kim, Youngrok; Choi, Barbara Yuri; Chung, Seungjun; Hong, Woong-Ki; Lee, Takhee

2016-11-10

We investigated the trap-mediated electronic transport properties of pentacene/molybdenum disulphide (MoS 2 ) p-n heterojunction devices. We observed that the hybrid p-n heterojunctions were gate-tunable and were strongly affected by trap-assisted tunnelling through the van der Waals gap at the heterojunction interfaces between MoS 2 and pentacene. The pentacene/MoS 2 p-n heterojunction diodes had gate-tunable high ideality factor, which resulted from trap-mediated conduction nature of devices. From the temperature-variable current-voltage measurement, a space-charge-limited conduction and a variable range hopping conduction at a low temperature were suggested as the gate-tunable charge transport characteristics of these hybrid p-n heterojunctions. Our study provides a better understanding of the trap-mediated electronic transport properties in organic/2-dimensional material hybrid heterojunction devices.

Dependence of Pentacene Crystal Growth on Dielectric Roughness for Fabrication of Flexible Field-Effect Transistors

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, H.; Yang, C; Kim, S

2010-01-01

The dependence of pentacene nanostructures on gate dielectric surfaces were investigated for flexible organic field-effect transistor (OFET) applications. Two bilayer types of polymer/aluminum oxide (Al{sub 2}O{sub 3}) gate dielectrics were fabricated on commercial Al foils laminated onto a polymer back plate. Some Al foils were directly used as gate electrodes, and others were smoothly polished by an electrolytic etching. These Al surfaces were then anodized and coated with poly({alpha}-methyl styrene) (PAMS). For PAMS/Al{sub 2}O{sub 3} dielectrics onto etched Al foils, surface roughness up to 1 nm could be reached, although isolated dimples with a lateral diameter of several micrometers weremore » still present. On PAMS/Al{sub 2}O{sub 3} dielectrics (surface roughness >40 nm) containing mechanical grooves of Al foil, average hole mobility ({mu}FET) of 50 nm thick pentacene-FETs under the low operating voltages (|V| < 6 V) was {approx}0.15 cm{sup 2} V{sup -1} s{sup -1}. In contrast, pentacene-FETs employing the etched Al gates exhibited {mu}FET of 0.39 cm{sup 2} V{sup -1} s{sup -1}, which was comparable to that of reference samples with PAMS/Al{sub 2}O{sub 3} dielectrics onto flat sputtered Al gates. Conducting-probe atomic force microscopy and two-dimensional X-ray diffraction of pentacene films with various thicknesses revealed different out-of-plane and in-plane crystal orderings of pentacene, depending on the surface roughness of the gate dielectrics.« less

Temperature-dependent field-effect carrier mobility in organic thin-film transistors with a gate SiO2 dielectric modified by H2O2 treatment

NASA Astrophysics Data System (ADS)

Lin, Yow-Jon; Hung, Cheng-Chun

2018-02-01

The effect of the modification of a gate SiO2 dielectric using an H2O2 solution on the temperature-dependent behavior of carrier transport for pentacene-based organic thin-film transistors (OTFTs) is studied. H2O2 treatment leads to the formation of Si(-OH) x (i.e., the formation of a hydroxylated layer) on the SiO2 surface that serves to reduce the SiO2 capacitance and weaken the pentacene-SiO2 interaction, thus increasing the field-effect carrier mobility ( µ) in OTFTs. The temperature-dependent behavior of carrier transport is dominated by the multiple trapping model. Note that H2O2 treatment leads to a reduction in the activation energy. The increased value of µ is also attributed to the weakening of the interactions of the charge carriers with the SiO2 dielectric that serves to reduce the activation energy.

Water-induced polaron formation at the pentacene surface: Quantum mechanical molecular mechanics simulations

NASA Astrophysics Data System (ADS)

Cramer, Tobias; Steinbrecher, Thomas; Koslowski, Thorsten; Case, David A.; Biscarini, Fabio; Zerbetto, Francesco

2009-04-01

Water is an omnipresent polar impurity that is expected to be the origin of many electric degradation phenomena observed in organic semiconductors. Here, we describe a microscopic model for polaron formation in the outermost layer of a pentacene crystal due to the polarization of a nearby water layer. The efficient coupling of a classical force field that describes the liquid with a tight-binding model that represents the π system of the organic layer permits the calculation of nanosecond length trajectories. The model predicts that the reorientation of water dipoles stabilizes positive charge carriers on average by 0.6 eV and thus leads to a polaron trap state at the liquid interface. Thermal fluctuations of the water molecules provoke two-dimensional diffusive hopping of the charge carrier parallel to the interface with mobilities of up to 0.6cm2s-1V-1 and lead to an amorphous broadening of the valence-band tail. As a consequence, water-filled nanocavities act as trapping sites in pentacene transistors. Instead, a complete wetting of the organic film is expected to result in fast thermally activated hopping transport. Polaron trapping is thus not expected to be a limiting factor for transistor-based sensors that operate under water.

Photocurrent spectroscopy of pentacene thin film transistors

NASA Astrophysics Data System (ADS)

Breban, Mihaela

We demonstrate the application of photocurrent modulation spectroscopy in characterizing the performance of organic thin-film transistors. A parallel analysis of the direct current and photocurrent voltage characteristics provides a model free determination of the field-effect mobility and the density of free carriers in the transistor channel as a function of the applied gate voltage. Applying this technique to pentacene thin-film transistors demonstrates that the mobility increases as V1/3g . The free-carrier density is approximately 1/10 of the expected capacitive charge, and the mobility increases monotonically with the free carrier density, consistent with the trap and release model of transport. Also, the modulated photocurrent spectroscopy can be used as a probe of defect states in pentacene thin film transistors, measuring simultaneously the magnitude and the phase of the photocurrent as a function of the modulation frequency. This is accomplished by modeling the photo-carrier generation process as exciton dissociation via interaction with localized traps. Experimental data reveal a Gaussian distribution of localized states centered around 0.3 eV above the highest occupied molecular orbital. We also investigated the effect of the gate dielectric material with our probe and found that the position of the extracted Gaussian slightly shifts, consistent with the expected image charge effect for Pn through the dielectric substrate. Also shifts in the Gaussian position for samples fabricated with variable deposition conditions are correlated with changes in Pn morphology. The morphological differences between Pn films were also detected in current-voltage characteristics and photocurrent spectra. However, the origin of the ubiquitous 0.3 eV defect in Pn seems to be unrelated to structural differences in Pn films.

Simulation Based Performance Comparison of Transistors Designed using Standard Photolithographic and Coarse Printing Design Specifications

DTIC Science & Technology

2010-01-01

between pentacene and parylene was considered for the simulation. The interface charges are supposed to be formed during the fabrication process of the...performed at T=300°K. Pentacene Band gap 2.2 eV Thickness 150 nm Affinity 2.7 eV Permittivity 3.0 Nc, Nv 2.4×1021 cm−3 Acceptor trap 2.4×1017 cm−3 μi 0.1 cm2...March 2010 Received in revised form 2 October 2010 Accepted 4 October 2010 Available online x Keywords: Photolithography Inkjet printing Pentacene

Defect states and their energetic position and distribution in organic molecular semiconductors

NASA Astrophysics Data System (ADS)

Sharma, Akanksha; Yadav, Sarita; Kumar, Pramod; Ray Chaudhuri, Sumita; Ghosh, Subhasis

2013-04-01

Energetic position and distribution of defect states due to structural disorder in pentacene and copper phthalocyanine have been obtained by capacitance based spectroscopic techniques. It has been shown that capacitance-frequency and capacitance-voltage characteristics exhibit Gaussian distribution of traps with an energetic position at around 0.5 eV above the highest occupied molecular orbital level of the pentacene and CuPc. These traps have been created by varying growth conditions and almost identical trap parameters in pentacene and copper phthalocyanine indicate that similar structural disorder is responsible for these traps.

Investigation of pentacene growth on SiO2 gate insulator after photolithography for nitrogen-doped LaB6 bottom-contact electrode formation

NASA Astrophysics Data System (ADS)

Maeda, Yasutaka; Hiroki, Mizuha; Ohmi, Shun-ichiro

2018-04-01

Nitrogen-doped (N-doped) LaB6 is a candidate material for the bottom-contact electrode of n-type organic field-effect transistors (OFETs). However, the formation of a N-doped LaB6 electrode affects the surface morphology of a pentacene film. In this study, the effects of surface treatments and a N-doped LaB6 interfacial layer (IL) were investigated to improve the pentacene film quality after N-doped LaB6 electrode patterning with diluted HNO3, followed by resist stripping with acetone and methanol. It was found that the sputtering damage during N-doped LaB6 deposition on a SiO2 gate insulator degraded the crystallinity of pentacene. The H2SO4 and H2O2 (SPM) and diluted HF treatments removed the damaged layer on the SiO2 gate insulator surface. Furthermore, the N-doped LaB6 IL improved the crystallinity of pentacene and realized dendritic grain growth. Owing to these surface treatments, the hole mobility improved from 2.8 × 10-3 to 0.11 cm2/(V·s), and a steep subthreshold swing of 78 mV/dec for the OFET with top-contact configuration was realized in air even after bottom-contact electrode patterning.

Thermally dried ink-jet process for 6,13-bis(triisopropylsilylethynyl)-pentacene for high mobility and high uniformity on a large area substrate

USGS Publications Warehouse

Ryu, Gi Seong; Lee, Myung Won; Jeong, Seung Hyeon; Song, Chung Kun

2012-01-01

In this study we developed a simple ink-jet process for 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS-pentacene), which is known as a high-mobility soluble organic semiconductor, to achieve relatively high-mobility and high-uniformity performance for large-area applications. We analyzed the behavior of fluorescent particles in droplets and applied the results to determining a method of controlling the behavior of TIPS-pentacene molecules. The grain morphology of TIPS-pentacene varied depending on the temperature applied to the droplets during drying. We were able to obtain large and uniform grains at 46 degrees C without any "coffee stain". The process was applied to a large-size organic thin-film transistor (OTFT) backplane for an electrophoretic display panel containing 192 x 150 pixels on a 6-in.-sized substrate. The average of mobilities of 36 OTFTs, which were taken from different locations of the backplane, was 0.44 +/- 0.08 cm2.V-1.s-1, with a small deviation of 20%, over a 6-in.-size area comprising 28,800 OTFTs. This process providing high mobility and high uniformity can be achieved by simply maintaining the whole area of the substrate at a specific temperature (46 degrees C in this case) during drying of the droplets.

Optimization of pentacene double floating gate memories based on charge injection regulated by SAM functionalization

NASA Astrophysics Data System (ADS)

Li, S.; Guérin, D.; Lenfant, S.; Lmimouni, K.

2018-02-01

Pentacene based double nano-floating gate memories (NFGM) by using gold nanoparticles (Au NPs) and reduced graphene oxide (rGO) sheets as charge trapping layers are prepared and demonstrated. Particularly, the NFGM chemically treated by 2,3,4,5,6-pentafluorobenzenethiol (PFBT) self-assembled monolayers (SAM) exhibits excellent memory performances, including high mobility of 0.23 cm2V-1s-1, the large memory window of 51 V, and the stable retention property more than 108 s. Comparing the performances of NFGM without treating with PFBT SAM, the improving performances of the memory devices by SAM modification are explained by the increase of charge injection, which could be further investigated by XPS and UPS. In particular, the results highlight the utility of SAM modulations and controlling of charge transport in the development of organic transistor memories.

Multifunctional graphene optoelectronic devices capable of detecting and storing photonic signals.

PubMed

Jang, Sukjae; Hwang, Euyheon; Lee, Youngbin; Lee, Seungwoo; Cho, Jeong Ho

2015-04-08

The advantages of graphene photodetectors were utilized to design a new multifunctional graphene optoelectronic device. Organic semiconductors, gold nanoparticles (AuNPs), and graphene were combined to fabricate a photodetecting device with a nonvolatile memory function for storing photonic signals. A pentacene organic semiconductor acted as a light absorption layer in the device and provided a high hole photocurrent to the graphene channel. The AuNPs, positioned between the tunneling and blocking dielectric layers, acted as both a charge trap layer and a plasmonic light scatterer, which enable storing of the information about the incident light. The proposed pentacene-graphene-AuNP hybrid photodetector not only performed well as a photodetector in the visible light range, it also was able to store the photonic signal in the form of persistent current. The good photodetection performance resulted from the plasmonics-enabled enhancement of the optical absorption and from the photogating mechanisms in the pentacene. The device provided a photoresponse that depended on the wavelength of incident light; therefore, the signal information (both the wavelength and intensity) of the incident light was effectively committed to memory. The simple process of applying a negative pulse gate voltage could then erase the programmed information. The proposed photodetector with the capacity to store a photonic signal in memory represents a significant step toward the use of graphene in optoelectronic devices.

Amorphous silicon and organic thin film transistors for electronic applications

NASA Astrophysics Data System (ADS)

Zhou, Lisong

Recently, flexible thin film electronics has attracted huge research interest, and as now, many prototypes are being developed and demonstrated by companies around the world, including displays, logic circuit, and solar cells. Flexible electronics offers many potential advantages: it can not only generate new functions like flexible displays or solar cells, also allow very low cost manufacturing through the use of cheap polymeric substrates and roll-to-roll fabrication. a-Si:H TFT fabrications are compatible with flexible polyimide substrate materials. With the interests in the space environment, for the first time, we tested the performance changes of flexible a-Si:H TFTs, on polyimide substrates, due to irradiation and mechanical stress. Significant changes were found on TFTs after irradiation with fast electrons, which, however, was essentially removed by post-irradiation thermal annealing. On the other hand, few changes were found in TFTs by mechanical stress. These preliminary results indicate that it can be readily engineered for space applications. Furthermore, for the first time, we designed and fabricated ungated n+ muC-Si and gated a-Si:H strain sensors on flexible polyimide substrates. Compared with commercial metallic foil strain sensors, ungated muC-Si sensors and gated a-Si:H sensors are two orders of magnitude smaller in area and consume two orders or magnitude less power. Integration with a-Si:H TFTs can also allow large arrays of strain sensors to be fabricated. To take advantage of lower glass-transition-temperature polymeric substrate materials, reduced processing temperature is desired. The 150°C low-temperature deposition process is achieved by using hydrogen dilution in the PECVD process. The TFT performance and bias stability property are tested similar to that of a 250°C process. These results suggest its viability for practical applications. For even lower process temperature, we have considered organic TFTs. As a practical demonstration, we integrated pentacene TFTs with OLEDs in a simple display. Pentacene TFT passivation techniques were researched, and a PVA and parylene bilayer structure was used. We designed and demonstrated 48 x 48-pixel active matrix OTFTOLED displays, and to our best knowledge, they are the largest on glass substrates and the first on flexible PET substrates. Device performance, uniformity and stability are also compared. These results demonstrate that pentacene TFTs are viable candidates for active-matrix OLED displays and other flexible electronics applications.

Tunable organic transistors that use microfluidic source and drain electrodes

NASA Astrophysics Data System (ADS)

Maltezos, George; Nortrup, Robert; Jeon, Seokwoo; Zaumseil, Jana; Rogers, John A.

2003-09-01

This letter describes a type of transistor that uses conducting fluidic source and drain electrodes of mercury which flow on top of a thin film of the organic semiconductor pentacene. Pumping the mercury through suitably designed microchannels changes the width of the transistor channel and, therefore, the electrical characteristics of the device. Measurements on transistors with a range of channel lengths reveal low contact resistances between mercury and pentacene. Data collected before, during, and after pumping the mercury through the microchannels demonstrate reversible and systematic tuning of the devices. This unusual type of organic transistor has the potential to be useful in plastic microfluidic devices that require active elements for pumps, sensors, or other components. It also represents a noninvasive way to build transistor test structures that incorporate certain classes of chemically and mechanically fragile organic semiconductors.

Hybrid Inorganic/Organic Photovoltaics: Translating Fundamental Nanostructure Research to Enhanced Solar Conversion Efficiency

DTIC Science & Technology

2008-12-31

component hybrid nanocrystals constituting pentacene or single wall carbon nanotube (SWCNT) as well as through control of interfacial chemistry and linkage...nanotubes-quantum dot conjugates or pentacene -quantum dot composits into organic matrices significantly improved photoconductivity of polymer/nanocrystal

A New Synthesis of Porphyrins with Extended Conjugation and their Photophysics

DTIC Science & Technology

2005-04-21

organic semiconductors for transistor applications comparable with pentacene . So more π-expanded systems, such as TAnPs, might be promising...44, 1856 (2005). (6) Photochemical synthesis of pentacene and its derivatives, H. Yamada, Y. Yamashita, M. Kikuchi, H. Watanabe, T. Okujima, H

Is Bare Band Description of Carrier Transport Appropriate in Pentacene?

NASA Astrophysics Data System (ADS)

Andersen, John D.; Giuggioli, Luca; Kenkre, V. M.

2002-03-01

Experiments on injected charges in pentacene single crystals reveal mobilities typical of inorganic semiconductors and temperature dependence (for T<430K) suggesting bandlike behavior.(J. H. Schon, C. Kloc, and B. Batlogg, Phys. Rev. Lett. 86, 3843 (2001)) Polaronic bands, particularly their narrowing with increasing temperature, were invoked(V. M. Kenkre, John D. Andersen, D.H. Dunlap, and C.B. Duke, Phys. Rev. Lett. 62, 1165 (1989)) in the related naphthalene problem.(L. B. Schein, C. B. Duke, and A.R. McGhie, Phys. Rev. Lett. 40, 197 (1978); L. B. Schein, W. Warta, and N. Karl, Chem. Phys. Lett. 100, 34 (1983)) Because the low temperature mobility values in pentacene suggest moderately large bandwidths, we address two questions. Does a bare wide (effectively infinite) band description work for pentacene for T<400K? And, is a bare finite band description compatible with those data? These questions are answered by modifications of a theory originally constructed for inorganic materials and a newly developed mobility theory.

Spin-dependent electrical conduction in a pentacene Schottky diode explored by electrically detected magnetic resonance

NASA Astrophysics Data System (ADS)

Fukuda, Kunito; Asakawa, Naoki

2017-02-01

Reported is the observation of dark spin-dependent electrical conduction in a Schottky barrier diode with pentacene (PSBD) using electrically detected magnetic resonance at room temperature. It is suggested that spin-dependent conduction exists in pentacene thin films, which is explored by examining the anisotropic linewidth of the EDMR signal and current density-voltage (J-V) measurements. The EDMR spectrum can be decomposed to Gaussian and Lorentzian components. The dependency of the two signals on the applied voltage was consistent with the current density-voltage (J-V) of the PSBD rather than that of the electron-only device of Al/pentacene/Al, indicating that the spin-dependent conduction is due to bipolaron formation associated with hole polaronic hopping processes. The applied-voltage dependence of the ratio of intensity of the Gaussian line to the Lorentzian may infer that increasing current density should make conducting paths more dispersive, thereby resulting in an increased fraction of the Gaussian line due to the higher dispersive g-factor.

Theory of Transient Excited State Absorptions in Pentacene and Derivatives: Triplet-Triplet Biexciton versus Free Triplets.

PubMed

Khan, Souratosh; Mazumdar, Sumit

2017-12-07

Recent experiments in several singlet-fission materials have found that the triplet-triplet biexciton either is the primary product of photoexcitation or has a much longer lifetime than believed until now. It thus becomes essential to determine the difference in the spectroscopic signatures of the bound triplet-triplet and free triplets to distinguish between them optically. We report calculations of excited state absorptions (ESAs) from the singlet and triplet excitons and from the triplet-triplet biexciton for a pentacene crystal with the herringbone structure and for nanocrystals of bis(triisopropylsilylethynyl) (TIPS)-pentacene. The triplet-triplet biexciton absorbs in both the visible and the near-infrared (NIR), while the monomer free triplet absorbs only in the visible. The intensity of the NIR absorption depends on the extent of intermolecular coupling, in agreement with observations in TIPS-pentacene nanocrystals. We predict additional weak ESA from the triplet-triplet but not from the triplet, at still lower energy.

Coupling between diffusion and orientation of pentacene molecules on an organic surface.

PubMed

Rotter, Paul; Lechner, Barbara A J; Morherr, Antonia; Chisnall, David M; Ward, David J; Jardine, Andrew P; Ellis, John; Allison, William; Eckhardt, Bruno; Witte, Gregor

2016-04-01

The realization of efficient organic electronic devices requires the controlled preparation of molecular thin films and heterostructures. As top-down structuring methods such as lithography cannot be applied to van der Waals bound materials, surface diffusion becomes a structure-determining factor that requires microscopic understanding. Scanning probe techniques provide atomic resolution, but are limited to observations of slow movements, and therefore constrained to low temperatures. In contrast, the helium-3 spin-echo (HeSE) technique achieves spatial and time resolution on the nm and ps scale, respectively, thus enabling measurements at elevated temperatures. Here we use HeSE to unveil the intricate motion of pentacene admolecules diffusing on a chemisorbed monolayer of pentacene on Cu(110) that serves as a stable, well-ordered organic model surface. We find that pentacene moves along rails parallel and perpendicular to the surface molecules. The experimental data are explained by admolecule rotation that enables a switching between diffusion directions, which extends our molecular level understanding of diffusion in complex organic systems.

JPRS Report, Science & Technology USSR: Physics & Mathematics.

DTIC Science & Technology

1991-01-17

Irregularities on Readings of Local Work Function by Scanning Tunneling Microscope [A.O. Golubok, N.A. Tarasov, et al; PISMA V ZHURNAL TEKHNICHESKOY...constant. The substances tested (anthracene, phenanthrene, naphthacene, triphenylene, p- terphenyl, pentacene , benzo(def)phenanthrene, benzo(ghl...in nucleus-nucleus collisions are analyzed, considering that local thermodynamic equilibrium establishes itself after two or three collisions to be

The Production of Polycyclic Aromatic Hydrocarbon Anions in Inert Gas Matrices Doped with Alkali Metals. Electronic Absorption Spectra of the Pentacene Anion (C22H14(-))

NASA Technical Reports Server (NTRS)

Halasinski, Thomas M.; Hudgins, Douglas M.; Salama, Farid; Allamandola, Louis J.; Mead, Susan (Technical Monitor)

1999-01-01

The absorption spectra of pentacene (C22H14) and its radical cation (C22H14(+)) and anion (C22H14(-)) isolated in inert-gas matrices of Ne, Ar, and Kr are reported from the ultraviolet to the near-infrared. The associated vibronic band systems and their spectroscopic assignments are discussed together with the physical and chemical conditions governing ion (and counterion) production in the solid matrix. In particular, the formation of isolated pentacene anions is found to be optimized in matrices doped with alkali metal (Na and K).

Spatial profile of charge storage in organic field-effect transistor nonvolatile memory using polymer electret

NASA Astrophysics Data System (ADS)

She, Xiao-Jian; Liu, Jie; Zhang, Jing-Yu; Gao, Xu; Wang, Sui-Dong

2013-09-01

Spatial profile of the charge storage in the pentacene-based field-effect transistor nonvolatile memories using poly(2-vinyl naphthalene) electret is probed. The electron trapping into the electret after programming can be space dependent with more electron storage in the region closer to the contacts, and reducing the channel length is an effective approach to improve the memory performance. The deficient electron supply in pentacene is proposed to be responsible for the inhomogeneous electron storage in the electret. The hole trapping into the electret after erasing is spatially homogeneous, arising from the sufficient hole accumulation in the pentacene channel.

Observation of Frenkel and charge transfer excitons in pentacene single crystals using spectroscopic generalized ellipsometry

NASA Astrophysics Data System (ADS)

Qi, Dongchen; Su, Haibin; Bastjan, M.; Jurchescu, O. D.; Palstra, T. M.; Wee, Andrew T. S.; Rübhausen, M.; Rusydi, A.

2013-09-01

We report on the emerging and admixture of Frenkel and charge transfer (CT) excitons near the absorption onset in pentacene single crystals. Using high energy-resolution spectroscopic generalized ellipsometry with in-plane polarization dependence, the excitonic nature of three lowest lying excitations is discussed. Their distinct polarization dependence strongly indicates the presence of both Frenkel and CT types of excitons near the excitation onset. In particular, the peculiar polarization behavior of the second excitation can only be rationalized by taking into account the inherent CT transition dipole moment. This observation has important implications for the pentacene-based optoelectronic devices.

Molecular control of pentacene/ZnO photoinduced charge transfer

NASA Astrophysics Data System (ADS)

Spalenka, Josef W.; Paoprasert, Peerasak; Franking, Ryan; Hamers, Robert J.; Gopalan, Padma; Evans, Paul G.

2011-03-01

Photoinduced charge transfer modifies the device properties of illuminated pentacene field effect transistors (FETs) incorporating ZnO quantum dots at the gate insulator/pentacene interface. The transferred charge is trapped on electronic states associated with the ZnO quantum dots, with a steady state population approximately proportional to the rate of organic-inorganic charge transfer. Trapped charge shifts the threshold voltage of the FETs, providing the means to evaluate the rate of organic/inorganic charge transfer and the effects of interface modification. Monolayers of the wide-gap alkane stearic acid and the conjugated oligomer terthiophene attached to the ZnO suppress or permit charge transfer, respectively.

Synthesis of Dibenzo[h,rst]pentaphenes and Dibenzo[fg,qr]pentacenes by the Chemoselective C-O Arylation of Dimethoxyanthraquinones.

PubMed

Suzuki, Yusuke; Yamada, Kohei; Watanabe, Kentaro; Kochi, Takuya; Ie, Yutaka; Aso, Yoshio; Kakiuchi, Fumitoshi

2017-07-21

A convenient method for the syntheses of dibenzo[h,rst]pentaphenes and dibenzo[fg,qr]pentacenes via the ruthenium-catalyzed chemoselective C-O arylation of 1,4- and 1,5-dimethoxyanthraquinones is described. Dimethoxyanthraquinones reacted selectively with arylboronates at the ortho C-O bonds to give diarylation products. An efficient two-step procedure consisting of a Corey-Chaykofsky reaction and subsequent dehydrative aromatization afforded derivatives of dibenzo[h,rst]pentaphenes and dibenzo[fg,qr]pentacenes. Hole-transporting characteristics were observed for a device with a bottom-contact configuration that was fabricated from one of these polycyclic aromatic hydrocarbons.

Thermally Dried Ink-Jet Process for 6,13-Bis(triisopropylsilylethynyl)-Pentacene for High Mobility and High Uniformity on a Large Area Substrate

NASA Astrophysics Data System (ADS)

Ryu, Gi Seong; Lee, Myung Won; Jeong, Seung Hyeon; Song, Chung Kun

2012-05-01

In this study we developed a simple ink-jet process for 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS-pentacene), which is known as a high-mobility soluble organic semiconductor, to achieve relatively high-mobility and high-uniformity performance for large-area applications. We analyzed the behavior of fluorescent particles in droplets and applied the results to determining a method of controlling the behavior of TIPS-pentacene molecules. The grain morphology of TIPS-pentacene varied depending on the temperature applied to the droplets during drying. We were able to obtain large and uniform grains at 46 °C without any “coffee stain”. The process was applied to a large-size organic thin-film transistor (OTFT) backplane for an electrophoretic display panel containing 192×150 pixels on a 6-in.-sized substrate. The average of mobilities of 36 OTFTs, which were taken from different locations of the backplane, was 0.44±0.08 cm2·V-1·s-1, with a small deviation of 20%, over a 6-in.-size area comprising 28,800 OTFTs. This process providing high mobility and high uniformity can be achieved by simply maintaining the whole area of the substrate at a specific temperature (46 °C in this case) during drying of the droplets.

3D reconstruction of pentacene structural organization in top-contact OTFTs via resonant soft X-ray reflectivity

NASA Astrophysics Data System (ADS)

Capelli, Raffaella; Nardi, Marco Vittorio; Toccoli, Tullio; Verucchi, Roberto; Dinelli, Franco; Gelsomini, Carolina; Koshmak, Konstantin; Giglia, Angelo; Nannarone, Stefano; Pasquali, Luca

2018-01-01

Herein, we describe the use of soft X-ray reflectivity at the carbon K-edge to study the molecular organization (orientation, structure, and morphology) of pentacene active films in a top-contact transistor geometry. This technique is not affected by sample charging, and it can be applied in the case of insulating substrates. In addition, the sampling depth is not limited to the near-surface region, giving access to buried device interfaces (metal/organic and dielectric/organic). Spectral lineshape simulations, based on ab-initio calculations using a realistic 3D layer-by-layer model, allow us to unravel the details of the molecular organization in all the specific and crucial areas of the active film, overcoming the limitations of conventional approaches. The tilt angle of the long molecular axis in the whole film is found to progressively decrease with respect to the substrate normal from 25° to 0° with the increasing film thickness. A full vertical alignment, optimal for in-plane charge hopping, is reached only after the complete formation of the first five monolayers. Remarkably, starting from the first one in contact with the dielectric substrate, all the monolayers in the stack show a change in orientation with the increasing thickness. On the other hand, at the buried interface with a gold top-contact, the molecules assume a flat orientation that only propagates for two or three monolayers into the organic film. Top-contact devices with the highest performances can thus be obtained using films of at least ten monolayers. This explains the observed thickness dependence of charge mobility in pentacene transistors.

Pentacene-based low voltage organic field-effect transistors with anodized Ta2O5 gate dielectric

NASA Astrophysics Data System (ADS)

Jeong, Yeon Taek; Dodabalapur, Ananth

2007-11-01

Pentacene-based low voltage organic field-effect transistors were realized using an anodized Ta2O5 gate dielectric. The Ta2O5 gate dielectric layer with a surface roughness of 1.3Å was obtained by anodizing an e-beam evaporated Ta film. The device exhibited values of saturation mobility, threshold voltage, and Ion/Ioff ratio of 0.45cm2/Vs, 0.56V, and 7.5×101, respectively. The gate leakage current was reduced by more than 70% with a hexamethyldisilazane (HMDS) treatment on the Ta2O5 layer. The HMDS treatment also resulted in enhanced mobility values and a larger pentacene grain size.

Two-Photon Absorption in Pentacene Dimers: The Importance of the Spacer Using Upconversion as an Indirect Route to Singlet Fission.

PubMed

Garoni, Eleonora; Zirzlmeier, Johannes; Basel, Bettina S; Hetzer, Constantin; Kamada, Kenji; Guldi, Dirk M; Tykwinski, Rik R

2017-10-11

In this proof of concept study, we show that intramolecular singlet fission (iSF) can be initiated from a singlet excited state accessed by two-photon absorption, rather than through a traditional route of direct one-photon excitation (OPE). Thus, iSF in pentacene dimers 2 and 3 is enabled through NIR irradiation at 775 nm, a wavelength where neither dimer exhibits linear absorption of light. The adamantyl and meta-phenylene spacers 2 and 3, respectively, are designed to feature superimposable geometries, which establishes that the electronic coupling between the two pentacenes is the significant structural feature that dictates iSF efficiency.

Investigation of Ultraviolet Light Curable Polysilsesquioxane Gate Dielectric Layers for Pentacene Thin Film Transistors.

PubMed

Shibao, Hideto; Nakahara, Yoshio; Uno, Kazuyuki; Tanaka, Ichiro

2016-04-01

Polysilsesquioxane (PSQ) comprising 3-methacryloxypropyl groups was investigated as an ultraviolet (UV)-light curable gate dielectric-material for pentacene thin film transistors (TFTs). The surface of UV-light cured PSQ films was smoother than that of thermally cured ones, and the pentacene layers deposited on the UV-Iight cured PSQ films consisted of larger grains. However, carrier mobility of the TFTs using the UV-light cured PSQ films was lower than that of the TFTs using the thermally cured ones. It was shown that the cross-linker molecules, which were only added to the UV-light cured PSQ films, worked as a major mobility-limiting factor for the TFTs.

Relative permittivity and Hubbard U of pentacene extracted from scanning tunneling microscopy studies of p-doped films

NASA Astrophysics Data System (ADS)

Ha, Sieu D.; Qi, Yabing; Kahn, Antoine

2010-08-01

Temperature-dependent I- V measurements determine that pentacene is effectively p-doped by tetrafluoro-tetracyanoquinodimethane (F 4-TCNQ). It has been shown by scanning tunneling microscopy (STM) that the donated hole is localized by the ionized dopant counter potential, and that the hole can be visualized [4]. Here, it is argued that the effect of the localized hole on STM images should depend on distance as 1/ ɛr, as per the Coulomb potential. By fitting line profiles of localized hole features to the Coulomb potential, it is shown that approximate values for the relative permittivity and Hubbard U of pentacene can be extracted.

Singlet fission in pentacene dimers

PubMed Central

Zirzlmeier, Johannes; Lehnherr, Dan; Coto, Pedro B.; Chernick, Erin T.; Casillas, Rubén; Basel, Bettina S.; Thoss, Michael; Tykwinski, Rik R.; Guldi, Dirk M.

2015-01-01

Singlet fission (SF) has the potential to supersede the traditional solar energy conversion scheme by means of boosting the photon-to-current conversion efficiencies beyond the 30% Shockley–Queisser limit. Here, we show unambiguous and compelling evidence for unprecedented intramolecular SF within regioisomeric pentacene dimers in room-temperature solutions, with observed triplet quantum yields reaching as high as 156 ± 5%. Whereas previous studies have shown that the collision of a photoexcited chromophore with a ground-state chromophore can give rise to SF, here we demonstrate that the proximity and sufficient coupling through bond or space in pentacene dimers is enough to induce intramolecular SF where two triplets are generated on one molecule. PMID:25858954

Transport limited interfacial carrier relaxation in a double-layer device investigated by time-resolved second harmonic generation and impedance spectroscopy

NASA Astrophysics Data System (ADS)

Zhang, Le; Taguchi, Dai; Li, Jun; Manaka, Takaaki; Iwamoto, Mitsumasa

2011-02-01

The interfacial carrier relaxation in an indium tin oxide/polyimide/pentacene/Au double-layer device was studied in both time and frequency domains by using time-resolved second harmonic generation (TR-SHG) and impedance spectroscopy (IS), respectively. Although both hole and electron injection into the pentacene layer and their accumulation at the pentacene/polyimide interface were revealed in TR-SHG, it was only observed in IS under the hole injection condition. The "contradiction" between the two methods for the same carrier relaxation process was explained on the basis of a model, transport limited interfacial carrier relaxation, in which the quasistatic state governs the one-directional carrier transport.

Charge relaxation and dynamics in organic semiconductors

NASA Astrophysics Data System (ADS)

Kwok, H. L.

2006-08-01

Charge relaxation in dispersive materials is often described in terms of the stretched exponential function (Kohlrausch law). The process can be explained using a "hopping" model which in principle, also applies to charge transport such as current conduction. This work analyzed reported transient photoconductivity data on functionalized pentacene single crystals using a geometric hopping model developed by B. Sturman et al and extracted values (or range of values) on the materials parameters relevant to charge relaxation as well as charge transport. Using the correlated disorder model (CDM), we estimated values of the carrier mobility for the pentacene samples. From these results, we observed the following: i) the transport site density appeared to be of the same order of magnitude as the carrier density; ii) it was possible to extract lower bound values on the materials parameters linked to the transport process; and iii) by matching the simulated charge decay to the transient photoconductivity data, we were able to refine estimates on the materials parameters. The data also allowed us to simulate the stretched exponential decay. Our observations suggested that the stretching index and the carrier mobility were related. Physically, such interdependence would allow one to demarcate between localized molecular interactions and distant coulomb interactions.

γ-Herringbone Polymorph of 6,13-Bis(trimethylsilylethynyl)pentacene: A Potential Material for Enhanced Hole Mobility.

PubMed

Bhat, Vinayak; Gopan, Gopika; Nair, Nanditha G; Hariharan, Mahesh

2018-04-06

The introduction of the trialkylsilylethynyl group to the acene core is known to predominantly transform the herringbone structure of pentacene to a slip-stacked packing. However, herein, the occurrence of an unforeseen polymorph of 6,13-bis(trimethylsilylethynyl)pentacene (TMS-pentacene), with an atypical γ-herringbone packing arrangement, is reported. Intermolecular noncovalent interactions in the γ-herringbone polymorph are determined from Hirshfeld surface and quantum theory of atoms-in-molecules (QTAIM) analyses. Furthermore, a comparative truncated symmetry-adapted perturbation theory (SAPT(0)) energy decomposition analysis discloses the role of exchange repulsions that govern molecular packing in the γ-herringbone polymorph. Moreover, the computationally predicted electronic coupling and anisotropic mobility reveal the possibility of enhanced hole transport (μ h =3.7 cm 2  V -1  s -1 ) in the γ-herringbone polymorph, in contrast to the reported polymorph with a hole mobility of μ h =0.1 cm 2  V -1  s -1 . © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

A flexible amorphous Bi(5)Nb(3)O(15) film for the gate insulator of the low-voltage operating pentacene thin-film transistor fabricated at room temperature.

PubMed

Cho, Kyung-Hoon; Seong, Tae-Geun; Choi, Joo-Young; Kim, Jin-Seong; Kwon, Jae-Hong; Shin, Sang-Il; Chung, Myung-Ho; Ju, Byeong-Kwon; Nahm, Sahn

2009-10-20

The amorphous Bi(5)Nb(3)O(15) film grown at room temperature under an oxygen-plasma sputtering ambient (BNRT-O(2) film) has a hydrophobic surface with a surface energy of 35.6 mJ m(-2), which is close to that of the orthorhombic pentacene (38 mJ m(-2)), resulting in the formation of a good pentacene layer without the introduction of an additional polymer layer. This film was very flexible, maintaining a high capacitance of 145 nF cm(-2) during and after 10(5) bending cycles with a small curvature radius of 7.5 mm. This film was optically transparent. Furthermore, the flexible, pentacene-based, organic thin-film transistors (OTFTs) fabricated on the poly(ether sulfone) substrate at room temperature using a BNRT-O(2) film as a gate insulator exhibited a promising device performance with a high field effect mobility of 0.5 cm(2) V(-1) s(-1), an on/off current modulation of 10(5), and a small subthreshold slope of 0.2 V decade(-1) under a low operating voltage of -5 V. This device also maintained a high carrier mobility of 0.45 cm(2) V(-1 )s(-1) during the bending with a small curvature radius of 9 mm. Therefore, the BNRT-O(2) film is considered a promising material for the gate insulator of the flexible, pentacene-based OTFT.

Accurate description of charged excitations in molecular solids from embedded many-body perturbation theory

NASA Astrophysics Data System (ADS)

Li, Jing; D'Avino, Gabriele; Duchemin, Ivan; Beljonne, David; Blase, Xavier

2018-01-01

We present a novel hybrid quantum/classical approach to the calculation of charged excitations in molecular solids based on the many-body Green's function G W formalism. Molecules described at the G W level are embedded into the crystalline environment modeled with an accurate classical polarizable scheme. This allows the calculation of electron addition and removal energies in the bulk and at crystal surfaces where charged excitations are probed in photoelectron experiments. By considering the paradigmatic case of pentacene and perfluoropentacene crystals, we discuss the different contributions from intermolecular interactions to electronic energy levels, distinguishing between polarization, which is accounted for combining quantum and classical polarizabilities, and crystal field effects, that can impact energy levels by up to ±0.6 eV. After introducing band dispersion, we achieve quantitative agreement (within 0.2 eV) on the ionization potential and electron affinity measured at pentacene and perfluoropentacene crystal surfaces characterized by standing molecules.

Applications of Nonlinear Hole Burning Spectroscopy.

DTIC Science & Technology

1987-08-31

benerate a spectral hole through the generation of phonons interacting with the local environment of the surrounding glass. The key advantage to this...phthalocyanine, porphine, octaethylporphine, tetraphenylporphine, pentacene , and perylene. The host materials included methyl tetrahydrofuran, n-octane, benzoic...polymethyl methacrylate doped with either pentacene or phthalocyanne. There were also a number of experimental difficulties that had to be addressed

Acceleration of Singlet Fission in an Aza-Derivative of TIPS-Pentacene.

PubMed

Herz, Julia; Buckup, Tiago; Paulus, Fabian; Engelhart, Jens; Bunz, Uwe H F; Motzkus, Marcus

2014-07-17

The influence of the carbon to nitrogen substitution on the photoinduced dynamics of TIPS-pentacene was investigated by ultrafast transient absorption measurements on spin-coated thin films in the visible and in the near-infrared spectral region. A global target analysis was performed to provide a detailed picture of the excited-state dynamics. We found that the chemical modification has a high impact on the triplet formation and leads to shorter dynamics; hence it speeds up the singlet fission process. A faster relaxation from the singlet into the triplet manifold implies a higher efficiency because other relaxation channels are avoided. The air-stable aza-derivatives have the potential to exceed the energy conversion efficiency of TIPS-pentacene.

Effect of In Situ Annealing Treatment on the Mobility and Morphology of TIPS-Pentacene-Based Organic Field-Effect Transistors.

PubMed

Yang, Fuqiang; Wang, Xiaolin; Fan, Huidong; Tang, Ying; Yang, Jianjun; Yu, Junsheng

2017-08-23

In this work, organic field-effect transistors (OFETs) with a bottom gate top contact structure were fabricated by using a spray-coating method, and the influence of in situ annealing treatment on the OFET performance was investigated. Compared to the conventional post-annealing method, the field-effect mobility of OFET with 60 °C in situ annealing treatment was enhanced nearly four times from 0.056 to 0.191 cm 2 /Vs. The surface morphologies and the crystallization of TIPS-pentacene films were characterized by optical microscope, atomic force microscope, and X-ray diffraction. We found that the increased mobility was mainly attributed to the improved crystallization and highly ordered TIPS-pentacene molecules.

Effect of In Situ Annealing Treatment on the Mobility and Morphology of TIPS-Pentacene-Based Organic Field-Effect Transistors

NASA Astrophysics Data System (ADS)

Yang, Fuqiang; Wang, Xiaolin; Fan, Huidong; Tang, Ying; Yang, Jianjun; Yu, Junsheng

2017-08-01

In this work, organic field-effect transistors (OFETs) with a bottom gate top contact structure were fabricated by using a spray-coating method, and the influence of in situ annealing treatment on the OFET performance was investigated. Compared to the conventional post-annealing method, the field-effect mobility of OFET with 60 °C in situ annealing treatment was enhanced nearly four times from 0.056 to 0.191 cm2/Vs. The surface morphologies and the crystallization of TIPS-pentacene films were characterized by optical microscope, atomic force microscope, and X-ray diffraction. We found that the increased mobility was mainly attributed to the improved crystallization and highly ordered TIPS-pentacene molecules.

High Stability Pentacene Transistors Using Polymeric Dielectric Surface Modifier.

PubMed

Wang, Xiaohong; Lin, Guangqing; Li, Peng; Lv, Guoqiang; Qiu, Longzhen; Ding, Yunsheng

2015-08-01

1,6-bis(trichlorosilyl)hexane (C6Cl), polystyrene (PS), and cross-linked polystyrene (CPS) were investigated as gate dielectric modified layers for high performance organic transistors. The influence of the surface energy, roughness and morphology on the charge transport of the organic thin-film transistors (OTFTs) was investigated. The surface energy and roughness both affect the grain size of the pentacene films which will control the charge carrier mobility of the devices. Pentacene thin-film transistors fabricated on the CPS modified dielectric layers exhibited charge carrier mobility as high as 1.11 cm2 V-1 s-1. The bias stress stability for the CPS devices shows that the drain current only decays 1% after 1530 s and the mobility never decreases until 13530 s.

Cumulative effects of electrode and dielectric surface modifications on pentacene-based transistors

NASA Astrophysics Data System (ADS)

Devynck, Mélanie; Tardy, Pascal; Wantz, Guillaume; Nicolas, Yohann; Vellutini, Luc; Labrugère, Christine; Hirsch, Lionel

2012-01-01

Surface modifications of the dielectric and the metal of pentacene-based field effect transistors using self-assembled monolayer (SAM) were studied. First, a low interfacial trap density and pentacene 2D-growth were favored by the nonpolar and low surface energy of octadecyltrichlorosilane-based SAM. This treatment leaded to increased mobility up to 0.4 cm2 V-1 s-1 and no observable hysteresis on transfer curves. Second, reduced hole injection barrier and contact resistance were achieved by fluorinated thiols deposited on gold contacts resulting in an increased mobility up to 0.6 cm2 V-1 s-1. Finally, a high mobility of 2.6 cm2 V-1 s-1 was achieved by cumulative effects of both treatments.

Fabrication of Organic Thin Film Transistors Using Layer-By-Layer Assembly (Preprint)

DTIC Science & Technology

2007-03-01

thin-film transistors ( TFTs ) have received considerable attention as a low- cost, light-weight, flexible alternative to traditional amorphous silicon...Previous studies have investigated the use of a number of materials for both the active layer and the gate dielectric in various TFT architectures. These...performance. Conjugated small molecules, such as pentacene, or polymers, such as poly(3- hexylthiophene), are commonly used as the active layer in organic TFT

Wave function delocalization and large-amplitude vibrations of helium on corrugated aromatic microsurfaces: tetracene.He and pentacene.He van der Waals complexes.

PubMed

Xu, Minzhong; Bacić, Zlatko

2007-08-09

We report accurate quantum three-dimensional calculations of highly excited intermolecular vibrational states of the van der Waals (vdW) complexes tetracene.He and pentacene.He in the S1 excited electronic state. The aromatic molecules were taken to be rigid and the intermolecular potential energy surfaces (IPESs) were modeled as a sum of atom-atom Lennard-Jones pair potentials. The IPESs are corrugated in the direction of the long (x) axis of the aromatic molecules, due to the presence of the symmetrically equivalent global double minimum for tetracene.He, and a triple minimum (central global minimum and two equivalent local minima) for pentacene.He, on each side of the aromatic plane. Both IPESs have two additional minor equivalent local minima further away from the center of the molecule. The vdW vibrational states analyzed in this work cover about 80% of the well depths of the IPESs. The mode coupling is generally weak for those states whose out-of-plane (z) mode is unexcited. However, the z-mode fundamental is strongly coupled to the short-axis (y) in-plane mode, so that the pure z-mode excitation could not be identified. The He atom exhibits large in-plane spatial delocalizaton already in the ground vdW vibrational state, which increases rapidly upon the excitation of the in-plane x and y modes, with little hindrance by the corrugation of the aromatic microsurfaces. For the vdW vibrational energies considered, the He atom spatial delocalization reaches Deltax and Deltay values of approximately 5 and 4 A, respectively, and is limited only by the finite size of the aromatic substrates. Side-crossing delocalization of the wave functions on both sides of the molecular plane is found at excitation energies >30 cm(-1), giving rise to the energy splittings of the pairs of states symmetric/antisymmetric with respect to the aromatic plane; the splittings show strong vdW vibrational mode specificity.

Unveiling Singlet Fission Mediating States in TIPS-pentacene and its Aza Derivatives.

PubMed

Herz, Julia; Buckup, Tiago; Paulus, Fabian; Engelhart, Jens U; Bunz, Uwe H F; Motzkus, Marcus

2015-06-25

Femtosecond pump-depletion-probe experiments were carried out in order to shed light on the ultrafast excited-state dynamics of triisopropylsilylethynyl (TIPS)-pentacene and two nitrogen-containing derivatives, namely, diaza-TIPS-pentacene and tetraaza-TIPS-pentacene. Measurements performed in the visible and near-infrared spectral range in combination with rate model simulations reveal that singlet fission proceeds via the extremely short-lived intermediate (1)TT state, which absorbs in the near-infrared spectral region only. The T1 → T3 transition probed in the visible region shows a rise time that comprises two components according to a consecutive reaction (S1 → (1)TT → T1). The incorporation of nitrogen atoms into the acene structure leads to shorter dynamics, but the overall triplet formation follows the same kinetic model. This is of particular importance, since experiments on tetraaza-TIPS-pentacene allow for investigation of the triplet state in the visible range without an overlapping singlet contribution. In addition, the pump-depletion-probe experiments show that the triplet absorption in the visible (T1 → T3) and near-infrared (T1 → T2) regions occurs from the same initial state, which was questioned in previous studies. Furthermore, an additional ultrafast transfer between the excited triplet states (T3 → T2) is identified, which is also in agreement with the rate model simulation. By applying depletion pulses, which are resonant with higher vibrational levels, we gain insight into internal vibrational energy redistribution processes within the triplet manifold. This additional information is of great relevance regarding the study of loss channels within these materials.

Epitaxially grown strained pentacene thin film on graphene membrane.

PubMed

Kim, Kwanpyo; Santos, Elton J G; Lee, Tae Hoon; Nishi, Yoshio; Bao, Zhenan

2015-05-06

Organic-graphene system has emerged as a new platform for various applications such as flexible organic photovoltaics and organic light emitting diodes. Due to its important implication in charge transport, the study and reliable control of molecular packing structures at the graphene-molecule interface are of great importance for successful incorporation of graphene in related organic devices. Here, an ideal membrane of suspended graphene as a molecular assembly template is utilized to investigate thin-film epitaxial behaviors. Using transmission electron microscopy, two distinct molecular packing structures of pentacene on graphene are found. One observed packing structure is similar to the well-known bulk-phase, which adapts a face-on molecular orientation on graphene substrate. On the other hand, a rare polymorph of pentacene crystal, which shows significant strain along the c-axis, is identified. In particular, the strained film exhibits a specific molecular orientation and a strong azimuthal correlation with underlying graphene. Through ab initio electronic structure calculations, including van der Waals interactions, the unusual polymorph is attributed to the strong graphene-pentacene interaction. The observed strained organic film growth on graphene demonstrates the possibility to tune molecular packing via graphene-molecule interactions. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Influence of Pentacene Interface Layer in ITO/α-NPD/Alq3/Al Organic Light Emitting Diodes by Time-Resolved Electric-Field-Induced Optical Second-Harmonic Generation Measurement.

PubMed

Oda, Yoshiaki; Sadakata, Atsuo; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2016-04-01

By using I-V, EL-V, displacement current measurement (DCM) and time-resolved electric-field-induced optical second-harmonic generation (TR-EFISHG) measurement, we studied the influence of interface pentacene layer inserted between ITO and a-NPD layers in ITO/α-NPD/Alq3/Al OLEDs. All experiments were carried out for the OLEDs with and without a pentacene interface layer. The I-V and EL-V measurements showed the decrease of operating voltage of EL, the DCM showed the lowering of inception voltage of carrier injection by inserting a pentacene interface layer. The TR-EFISHG measurement showed the faster accumulation of holes at the interface between the a-NPD and Alq3 layers, which resulted in the relaxation of electric field of a-NPD layer accomplished by the increase of the conductivity and the increase of the electric field in the Alq3 layer. We conclude that TR-EFISHG measurement is helpful for understanding I-V and EL-V characteristics, and can be combined with other methods to give significant information which are impacted by the interface layer.

Effects of V2O5/Au bi-layer electrodes on the top contact Pentacene-based organic thin film transistors

NASA Astrophysics Data System (ADS)

Borthakur, Tribeni; Sarma, Ranjit

2017-05-01

Top-contact Pentacene-based organic thin film transistors (OTFTs) with a thin layer of Vanadium Pent-oxide between Pentacene and Au layer are fabricated. Here we have found that the devices with V2O5/Au bi-layer source-drain electrode exhibit better field-effect mobility, high on-off ratio, low threshold voltage and low sub-threshold slope than the devices with Au only. The field-effect mobility, current on-off ratio, threshold voltage and sub-threshold slope of V2O5/Au bi-layer OTFT estimated from the device with 15 nm thick V2O5 layer is .77 cm2 v-1 s-1, 7.5×105, -2.9 V and .36 V/decade respectively.

Isolated molecular dopants in pentacene observed by scanning tunneling microscopy

NASA Astrophysics Data System (ADS)

Ha, Sieu D.; Kahn, Antoine

2009-11-01

Doping is essential to the control of electronic structure and conductivity of semiconductor materials. Whereas doping of inorganic semiconductors is well established, doping of organic molecular semiconductors is still relatively poorly understood. Using scanning tunneling microscopy, we investigate, at the molecular scale, surface and subsurface tetrafluoro-tetracyanoquinodimethane p -dopants in the prototypical molecular semiconductor pentacene. Surface dopants diffuse to pentacene vacancies and appear as negatively charged centers, consistent with the standard picture of an ionized acceptor. Subsurface dopants, however, have the effect of a positive charge, evidence that the donated hole is localized by the parent acceptor counterion, in contrast to the model of doping in inorganic semiconductors. Scanning tunneling spectroscopy shows that the electron potential energy is locally lowered near a subsurface dopant feature, in agreement with the localized hole model.

A temperature dependent study on charge dynamics in organic molecular device: Effect of shallow traps on space charge limited behavior

NASA Astrophysics Data System (ADS)

Mukherjee, A. K.; Kavala, A. K.

2014-04-01

Shallow traps play a significant role in influencing charge dynamics through organic molecular thin films, such as pentacene. Sandwich cells of pentacene capped by gold electrodes are an excellent specimen to study the nature of underlying charge dynamics. In this paper, self-consistent numerical simulation of I-V characteristics is performed at various temperatures. The results have revealed negative value of Poole Frenkel coefficient. The location of trap energy level is found to be located at 0.24 eV above the highest occupied molecular orbit (HOMO) level of pentacene. Other physical parameters related to trap levels, such as density of states due to traps and effective carrier density due to traps, have also been estimated in this study.

Singlet exciton fission in polycrystalline pentacene: from photophysics toward devices.

PubMed

Wilson, Mark W B; Rao, Akshay; Ehrler, Bruno; Friend, Richard H

2013-06-18

Singlet exciton fission is the process in conjugated organic molecules bywhich a photogenerated singlet exciton couples to a nearby chromophore in the ground state, creating a pair of triplet excitons. Researchers first reported this phenomenon in the 1960s, an event that sparked further studies in the following decade. These investigations used fluorescence spectroscopy to establish that exciton fission occurred in single crystals of several acenes. However, research interest has been recently rekindled by the possibility that singlet fission could be used as a carrier multiplication technique to enhance the efficiency of photovoltaic cells. The most successful architecture to-date involves sensitizing a red-absorbing photoactive layer with a blue-absorbing material that undergoes fission, thereby generating additional photocurrent from higher-energy photons. The quest for improved solar cells has spurred a drive to better understand the fission process, which has received timely aid from modern techniques for time-resolved spectroscopy, quantum chemistry, and small-molecule device fabrication. However, the consensus interpretation of the initial studies using ultrafast transient absorption spectroscopy was that exciton fission was suppressed in polycrystalline thin films of pentacene, a material that would be otherwise expected to be an ideal model system, as well as a viable candidate for fission-sensitized photovoltaic devices. In this Account, we review the results of our recent transient absorption and device-based studies of polycrystalline pentacene. We address the controversy surrounding the assignment of spectroscopic features in transient absorption data, and illustrate how a consistent interpretation is possible. This work underpins our conclusion that singlet fission in pentacene is extraordinarily rapid (∼80 fs) and is thus the dominant decay channel for the photoexcited singlet exciton. Further, we discuss our demonstration that triplet excitons generated via singlet fission in pentacene can be dissociated at an interface with a suitable electron acceptor, such as fullerenes and infrared-absorbing inorganic semiconducting quantum dots. We highlight our recent reports of a pentacene/PbSe hybrid solar cell with a power conversion efficiency of 4.7% and of a pentacene/PbSe/amorphous silicon photovoltaic device. Although substantive challenges remain, both to better our understanding of the mechanism of singlet exciton fission and to optimize device performance, this realization of a solar cell where photocurrent is simultaneously contributed from a blue-absorbing fission-capable material and an infrared-absorbing conventional cell is an important step towards a dual-bandgap, single-junction, fission-enhanced photovoltaic device, which could one day surpass the Shockley-Queisser limit.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liguori, R.; Aprano, S.; Rubino, A.

In this study we analyzed one of the environmental factors that could affect organic materials. Pentacene thin film samples were fabricated and the degradation of their electrical characteristics was measured when the devices were exposed to ultraviolet light irradiation. The results have been reported in terms of a trap density model, which provides a description of the dynamics of light induced electrically active defects in an organic semiconductor.

Electron and hole transport in ambipolar, thin film pentacene transistors

NASA Astrophysics Data System (ADS)

Saudari, Sangameshwar R.; Kagan, Cherie R.

2015-01-01

Solution-processed, ambipolar, thin-film pentacene field-effect transistors were employed to study both electron and hole transport simultaneously in a single, organic solid-state device. Electron and hole mobilities were extracted from the respective unipolar saturation regimes and show thermally activated behavior and gate voltage dependence. We fit the gate voltage dependent saturation mobility to a power law to extract the characteristic Meyer-Neldel (MN) energy, a measure of the width of the exponential distribution of localized states extending into the energy gap of the organic semiconductor. The MN energy is ˜78 and ˜28 meV for electrons and holes, respectively, which reflects a greater density of localized tail states for electrons than holes. This is consistent with the lower measured electron than hole mobility. For holes, the well-behaved linear regime allows for four-point probe measurement of the contact resistance independent mobility and separate characterization of the width of the localized density of states, yielding a consistent MN energy of 28 meV.

Singlet exciton fission photovoltaics.

PubMed

Lee, Jiye; Jadhav, Priya; Reusswig, Philip D; Yost, Shane R; Thompson, Nicholas J; Congreve, Daniel N; Hontz, Eric; Van Voorhis, Troy; Baldo, Marc A

2013-06-18

Singlet exciton fission, a process that generates two excitons from a single photon, is perhaps the most efficient of the various multiexciton-generation processes studied to date, offering the potential to increase the efficiency of solar devices. But its unique characteristic, splitting a photogenerated singlet exciton into two dark triplet states, means that the empty absorption region between the singlet and triplet excitons must be filled by adding another material that captures low-energy photons. This has required the development of specialized device architectures. In this Account, we review work to develop devices that harness the theoretical benefits of singlet exciton fission. First, we discuss singlet fission in the archetypal material, pentacene. Pentacene-based photovoltaic devices typically show high external and internal quantum efficiencies. They have enabled researchers to characterize fission, including yield and the impact of competing loss processes, within functional devices. We review in situ probes of singlet fission that modulate the photocurrent using a magnetic field. We also summarize studies of the dissociation of triplet excitons into charge at the pentacene-buckyball (C60) donor-acceptor interface. Multiple independent measurements confirm that pentacene triplet excitons can dissociate at the C60 interface despite their relatively low energy. Because triplet excitons produced by singlet fission each have no more than half the energy of the original photoexcitation, they limit the potential open circuit voltage within a solar cell. Thus, if singlet fission is to increase the overall efficiency of a solar cell and not just double the photocurrent at the cost of halving the voltage, it is necessary to also harvest photons in the absorption gap between the singlet and triplet energies of the singlet fission material. We review two device architectures that attempt this using long-wavelength materials: a three-layer structure that uses long- and short-wavelength donors and an acceptor and a simpler, two-layer combination of a singlet-fission donor and a long-wavelength acceptor. An example of the trilayer structure is singlet fission in tetracene with copper phthalocyanine inserted at the C60 interface. The bilayer approach includes pentacene photovoltaic cells with an acceptor of infrared-absorbing lead sulfide or lead selenide nanocrystals. Lead selenide nanocrystals appear to be the most promising acceptors, exhibiting efficient triplet exciton dissociation and high power conversion efficiency. Finally, we review architectures that use singlet fission materials to sensitize other absorbers, thereby effectively converting conventional donor materials to singlet fission dyes. In these devices, photoexcitation occurs in a particular molecule and then energy is transferred to a singlet fission dye where the fission occurs. For example, rubrene inserted between a donor and an acceptor decouples the ability to perform singlet fission from other major photovoltaic properties such as light absorption.

Unified model for singlet fission within a non-conjugated covalent pentacene dimer

NASA Astrophysics Data System (ADS)

Basel, Bettina S.; Zirzlmeier, Johannes; Hetzer, Constantin; Phelan, Brian T.; Krzyaniak, Matthew D.; Reddy, S. Rajagopala; Coto, Pedro B.; Horwitz, Noah E.; Young, Ryan M.; White, Fraser J.; Hampel, Frank; Clark, Timothy; Thoss, Michael; Tykwinski, Rik R.; Wasielewski, Michael R.; Guldi, Dirk M.

2017-05-01

When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron-hole pairs, leading to a predicted ~50% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state that precedes formation of the pentacene triplet excitons. Using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.

Unified model for singlet fission within a non-conjugated covalent pentacene dimer.

PubMed

Basel, Bettina S; Zirzlmeier, Johannes; Hetzer, Constantin; Phelan, Brian T; Krzyaniak, Matthew D; Reddy, S Rajagopala; Coto, Pedro B; Horwitz, Noah E; Young, Ryan M; White, Fraser J; Hampel, Frank; Clark, Timothy; Thoss, Michael; Tykwinski, Rik R; Wasielewski, Michael R; Guldi, Dirk M

2017-05-18

When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron-hole pairs, leading to a predicted ∼50% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state that precedes formation of the pentacene triplet excitons. Using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.

Surface crystallographic structures of cellulose nanofiber films and overlayers of pentacene

NASA Astrophysics Data System (ADS)

Nakayama, Yasuo; Mori, Toshiaki; Tsuruta, Ryohei; Yamanaka, Soichiro; Yoshida, Koki; Imai, Kento; Koganezawa, Tomoyuki; Hosokai, Takuya

2018-03-01

Cellulose nanofibers or nanocellulose is a promising recently developed biomass and biodegradable material used for various applications. In order to utilize this material as a substrate in organic electronic devices, thorough understanding of the crystallographic structures of the surfaces of the nanocellulose composites and of their interfaces with organic semiconductor molecules is essential. In this work, surface crystallographic structures of nanocellulose films (NCFs) and overlayers of pentacene were investigated by two-dimensional grazing-incidence X-ray diffraction. The NCFs are found to crystallize on solid surfaces with the crystal lattice preserving the same structure of the known bulk phase, whereas distortion of interchain packing toward the surface normal direction is suggested. The pentacene overlayers on the NCFs are found to form the thin-film phase with an in-plane mean crystallite size of over 10 nm.

High-Yield Excited Triplet States in Pentacene Self-Assembled Monolayers on Gold Nanoparticles through Singlet Exciton Fission.

PubMed

Kato, Daiki; Sakai, Hayato; Tkachenko, Nikolai V; Hasobe, Taku

2016-04-18

One of the major drawbacks of organic-dye-modified self-assembled monolayers on metal nanoparticles when employed for efficient use of light energy is the fact that singlet excited states on dye molecules can be easily deactivated by means of energy transfer to the metal surface. In this study, a series of 6,13-bis(triisopropylsilylethynyl)pentacene-alkanethiolate monolayer protected gold nanoparticles with different particle sizes and alkane chain lengths were successfully synthesized and were employed for the efficient generation of excited triplet states of the pentacene derivatives by singlet fission. Time-resolved transient absorption measurements revealed the formation of excited triplet states in high yield (172±26 %) by suppressing energy transfer to the gold surface. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Engineering the mobility increment in pentacene-based field-effect transistors by fast cooling of polymeric modification layer

NASA Astrophysics Data System (ADS)

Ling, Haifeng; Zhang, Chenxi; Chen, Yan; Shao, Yaqing; Li, Wen; Li, Huanqun; Chen, Xudong; Yi, Mingdong; Xie, Linghai; Huang, Wei

2017-06-01

In this work, we investigate the effect of the cooling rate of polymeric modification layers (PMLs) on the mobility improvement of pentacene-based organic field-effect transistors (OFETs). In contrast to slow cooling (SC), the OFETs fabricated through fast cooling (FC) with PMLs containing side chain-phenyl rings, such as polystyrene (PS) and poly (4-vinylphenol) (PVP), show an obvious mobility incensement compared with that of π-group free polymethylmethacrylate (PMMA). Atomic force microscopy (AFM) images and x-ray diffraction (XRD) characterizations have showed that fast-cooled PMLs could effectively enhance the crystallinity of pentacene, which might be related to the optimized homogeneity of surface energy on the surface of polymeric dielectrics. Our work has demonstrated that FC treatment could be a potential strategy for performance modulation of OFETs.

Inherent structures of crystalline pentacene

NASA Astrophysics Data System (ADS)

Della Valle, Raffaele Guido; Venuti, Elisabetta; Brillante, Aldo; Girlando, Alberto

2003-01-01

Using a quasi-Monte Carlo scheme, we search the potential energy surface of crystalline pentacene to sample its local minima, which represent the "inherent" structures, i.e., the possible configurations of mechanical equilibrium. The system is described in terms of rigid molecules interacting through a standard atom-atom potential model. Several hundreds of distinct minima are encountered, with a surprising variety of structural arrangements. We find that deep minima are easily accessible because they exhibit a favorable energy distribution and their attraction basins tend to be wide. Thanks to these features of the potential surface, the localization the global minimum becomes entirely feasible, allowing reliable a priori predictions of the crystallographic structures. The results for pentacene are very satisfactory. In fact, the two deepest minima correspond to the structures of the two known experimental polymorphs, which are described correctly. Further polymorphs are also likely to exist.

Optical Detection and Spectroscopy of Single Molecules in a Solid.

DTIC Science & Technology

1989-03-23

the optical absorption spectrum of single dopant molecules of pentacene in a p-terphenyl host crystal at liquid-helium temperatures. To achieve this...dopant molecules of pentacene in a p-terphenyl host crystal at liquid-helium temperatures. To achieve this, frequency-modulation spectroscopy was combined...solid would provide an important new tool for the study of local absorber-host interactions that would be uncomplicated by the normal averaging over

Electron Transporting Semiconductor Dielectric Intramolecular

DTIC Science & Technology

2012-04-27

gate dielectric, and the capacitance times mobility was 80 nS/V (10x typical pentacene /oxide), stable to heating to 70 °C in air. Remarkably...oxide/ Pentacene Bilayer Transistors: High Mobility n-Channel, Ambipolar and Nonvolatile Devices” Adv. Funct. Mater. 18, 1832-1839 (2008) Sun, J...case of layered OSC OFETs. This proposal is somewhat different from a model by deLeeuw for amorphous OFETs13 in which carriers would be locally

Statistical Fine Structure in Inhomogeneously Broadened Absorption Lines in Solids.

DTIC Science & Technology

1987-12-22

the inhomogeneously broadened zero-phonon SijSo (0-0) absorption of pentacene molecules in crystals of p-terphenyl at liquid helium temperatures. SFS...structure (SFS) in the inhomogeneously broadened zero-phonon S, +- So (0-0) absorption of pentacene molecules in crystals of p-terphenyl at liquid helium...tile large multiplicity of local environments. Inhomogeneously broadened absorption lines are usually treated as smooth, Gaussian profiles. In recent

Organic Field Effect Transistors for Large Format Electronics

DTIC Science & Technology

2003-06-19

calculated output characteristics for a p-channel substrate insulator Organic layer Source Drain Gate 6 pentacene OFET with 2µm source to drain spacing...conventional transistors. Figure 3. Calculated output characteristics of a pentacene OFET with image charge induced contact barrier...Cross section view of a part of an OFET in the vicinity of a source or drain contact. local ordering due to surface energy effects. The development of

Ultrasensitive Laser Spectroscopy in Solids: Single-Molecule Detection

DTIC Science & Technology

1989-10-25

spite of detection intensity constraints necessary to avoid power broadening, the optical absorption spectrum of single molecules of pentacene In p...molecule detection, or SMD) would provide a useful tool for the study of local host-absorber interactions where tihe absorbing ,ontor is essentially at...modulation techniques 7. 8 for the model system composed of pentacene substitutional impurities in p-terphenyl crystals at 1.5K. The pontacene molecules can

High Performance Vertical Organic Field Effect Transistors

DTIC Science & Technology

2010-05-01

systems. In pentacene /C60 bilayer system, [4] we showed that both the disordered structure of C60 and the charge trapping effect at the C60...much less significant than that by charge trapping at the interface. We also demonstrated that blending CdTe nanoparticles into a polymer–fullerene...for space applications b. We studied the photomultiplication effect in both evaporated ( pentacene /C60 bilayer) and bulk- heterojunction donor/acceptor

Dynamic nuclear polarisation via the integrated solid effect II: experiments on naphthalene-h8 doped with pentacene-d14

NASA Astrophysics Data System (ADS)

Eichhorn, T. R.; van den Brandt, B.; Hautle, P.; Henstra, A.; Wenckebach, W. Th.

2014-07-01

In dynamic nuclear polarisation (DNP), also called hyperpolarisation, a small amount of unpaired electron spins is added to the sample containing the nuclear spins, and the polarisation of these unpaired electron spins is transferred to the nuclear spins by means of a microwave field. Traditional DNP polarises the electron spin of stable paramagnetic centres by cooling down to low temperature and applying a strong magnetic field. Then weak continuous wave microwave fields are used to induce the polarisation transfer. Complicated cryogenic equipment and strong magnets can be avoided using short-lived photo-excited triplet states that are strongly aligned in the optical excitation process. However, a much faster transfer of the electron spin polarisation is needed and pulsed DNP methods like nuclear orientation via electron spin locking (NOVEL) and the integrated solid effect (ISE) are used. To describe the polarisation transfer with the strong microwave fields in NOVEL and ISE, the usual perturbation methods cannot be used anymore. In the previous paper, we presented a theoretical approach to calculate the polarisation transfer in ISE. In the present paper, the theory is applied to the system naphthalene-h8 doped with pentacene-d14 yielding the photo-excited triplet states and compared with experimental results.

Nonvolatile memory thin film transistors using CdSe/ZnS quantum dot-poly(methyl methacrylate) composite layer formed by a two-step spin coating technique

NASA Astrophysics Data System (ADS)

Chen, Ying-Chih; Huang, Chun-Yuan; Yu, Hsin-Chieh; Su, Yan-Kuin

2012-08-01

The nonvolatile memory thin film transistors (TFTs) using a core/shell CdSe/ZnS quantum dot (QD)-poly(methyl methacrylate) (PMMA) composite layer as the floating gate have been demonstrated, with the device configuration of n+-Si gate/SiO2 insulator/QD-PMMA composite layer/pentacene channel/Au source-drain being proposed. To achieve the QD-PMMA composite layer, a two-step spin coating technique was used to successively deposit QD-PMMA composite and PMMA on the insulator. After the processes, the variation of crystal quality and surface morphology of the subsequent pentacene films characterized by x-ray diffraction spectra and atomic force microscopy was correlated to the two-step spin coating. The crystalline size of pentacene was improved from 147.9 to 165.2 Å, while the degree of structural disorder was decreased from 4.5% to 3.1% after the adoption of this technique. In pentacene-based TFTs, the improvement of the performance was also significant, besides the appearances of strong memory characteristics. The memory behaviors were attributed to the charge storage/discharge effect in QD-PMMA composite layer. Under the programming and erasing operations, programmable memory devices with the memory window (Δ Vth) = 23 V and long retention time were obtained.

Sharp organic interface of molecular C60 chains and a pentacene derivative SAM on Au(788): A combined STM & DFT study

NASA Astrophysics Data System (ADS)

Wang, Jun; Tang, Jian-Ming; Larson, Amanda M.; Miller, Glen P.; Pohl, Karsten

2013-12-01

Controlling the molecular structure of the donor-acceptor interface is essential to overcoming the efficiency bottleneck in organic photovoltaics. We present a study of self-assembled fullerene (C60) molecular chains on perfectly ordered 6,13-dichloropentacene (DCP) monolayers forming on a vicinal Au(788) surface using scanning tunneling microscopy in conjunction with density functional theory calculations. DCP is a novel pentacene derivative optimized for photovoltaic applications. The molecules form a brick-wall patterned centered rectangular lattice with the long axis parallel to the monatomic steps that separate the 3.9 nm wide Au(111) terraces. The strong interaction between the C60 molecules and the gold substrate is well screened by the DCP monolayer. At submonolayer C60 coverage, the fullerene molecules form long parallel chains, 1.1 nm apart, with a rectangular arrangement instead of the expected close-packed configuration along the upper step edges. The perfectly ordered DCP structure is unaffected by the C60 chain formation. The controlled sharp highly-ordered organic interface has the potential to improve the conversion efficiency in organic photovoltaics.

Charge transfer at organic-organic heterojunctions, and remote doping of a pentacene transistor

NASA Astrophysics Data System (ADS)

Zhao, Wei

Organic-organic heterojunctions (OOHs) are the fundamental building blocks of organic devices, such as organic light-emitting diodes, organic photovoltaic cells, and photo detectors. Transport of free electrons and holes, exciton formation, recombination or dissociation, and various other physical processes all take place in OOHs. Understanding the electronic structures of OOH is critical for studying device physics and further improving the performance of organic devices. This work focuses on the electronic structure, i.e., the energy level alignment, at OOHs, investigated by ultraviolet and inverse photoemission spectroscopy (UPS and IPES). The weak interaction that generally prevails at OOH interfaces leads to small interface dipoles of 0˜0.5eV. The experimental observations on the majority of OOHs studied can be semi-quantitatively predicted by the model derived from the induced density of interface states and charge neutrality level (IDIS/CNL). However, we also find that the electronic structure of interfaces between two small-band-gap semiconductors, e.g., using copper phthalocyanine (CuPc) as the donor and a tris(thieno)-hexaazatriphenylene derivative (THAP) as the acceptor, is strongly influenced by changes in the substrate work function. In these cases, the charge transfer that takes place at the interface is governed by thermodynamic equilibrium, dominating any subtle interaction due to IDIS/CNL. The impact of doping on the energy level alignment of OOHs is also studied. The charges donated by the dopant molecules transfer from the parent doped layer to the adjacent undoped layer, taking advantage of the molecular level offset, and are then spatially separated from the dopant molecules. Remote doping, based on this charge transfer mechanism, is demonstrated with the heterojunction formed between pentacene and N,N'-diphenyl-N,N'-bis(1-naphthyl)-1,1'bisphenyl-4,4'diazine (alpha-NPD) p-doped with tris[1,2-bis(trifluoromethyl) ethane-1,2-dithiolene] (Mo(tfd)3). A remotely doped pentacene transistor, based on this type of hetero-structure, exhibits increased conductivity, decreased activation energy for carrier hopping, and enhanced mobility, compared to an undoped transistor. Another featured improvement of the remotely doped transistor is that it can be reasonably switched off by placing an undoped interlayer in the structure. Our preliminary results show chemical doping technology can potentially benefit the organic thin film transistors.

The thermodynamic effects of ligand structure on the molecular recognition of mononuclear ruthenium polypyridyl complexes with B-DNA

USDA-ARS?s Scientific Manuscript database

The ruthenium(II) polypyridyl complexes (RPCs), [(phen)2Ru(tatpp)]Cl2 (3Cl2) and [(phen)2Ru (tatpp)Ru(phen)2]Cl4 (4Cl4), containing the large planar and redox-active tetraazatetrapyrido- pentacene (tatpp) ligand, cleave DNA in the presence of reducing agents in cell-free assays and show significant...

Persistant Spectral Hole-Burning: Photon-Gating and Fundamental Statistical Limits

DTIC Science & Technology

1989-11-03

pentacene inhomogeneous line that results from tile statistics of independent, additive random variables. For this data, Nil - 10’. The rms amplitude...features in inhomogencous lines. To illustrate this, Figure 5 shows a portion of the optical spectrum of pentacene in p-terphenyl before and after a...contained in each irradiated spot of recording medium. The stress-induced variations in the local environment of the storage centers are random in nature

Low leakage current gate dielectrics prepared by ion beam assisted deposition for organic thin film transistors

NASA Astrophysics Data System (ADS)

Kim, Chang Su; Jo, Sung Jin; Kim, Jong Bok; Ryu, Seung Yoon; Noh, Joo Hyon; Baik, Hong Koo; Lee, Se Jong; Kim, Youn Sang

2007-12-01

This communication reports on the fabrication of low operating voltage pentacene thin-film transistors with high-k gate dielectrics by ion beam assisted deposition (IBAD). These densely packed dielectric layers by IBAD show a much lower level of leakage current than those created by e-beam evaporation. These results, from the fact that those thin films deposited with low adatom mobility, have an open structure, consisting of spherical grains with pores in between, that acts as a significant path for leakage current. By contrast, our results demonstrate the potential to limit this leakage. The field effect mobility, on/off current ratio, and subthreshold slope obtained from pentacene thin-film transistors (TFTs) were 1.14 cm2/V s, 105, and 0.41 V/dec, respectively. Thus, the high-k gate dielectrics obtained by IBAD show promise in realizing low leakage current, low voltage, and high mobility pentacene TFTs.

Fabrication of InP-pentacene inorganic-organic hybrid heterojunction using MOCVD grown InP for photodetector application

NASA Astrophysics Data System (ADS)

Sarkar, Kalyan Jyoti; Pal, B.; Banerji, P.

2018-04-01

We fabricated inorganic-organic hybrid heterojunction between indium phosphide (InP) and pentacene for photodetector application. InP layer was grown on n-Si substrate by atmospheric pressure metal organic chemical vapour deposition (MOCVD) technique. Morphological properties of InP and pentacene thin film were characterized by atomic force microscopy (AFM). Current-voltage characteristics were investigated in dark and under illumination condition at room temperature. During illumination, different wavelengths of visible and infrared light source were employed to perform the electrical measurement. Enhancement of photocurrent was observed with decreasing in wavelength of incident photo radiation. Ideality factor was found to be 1.92. High rectification ratio of 225 was found at ± 3 V in presence of infrared light source. This study provides new insights of inorganic-organic hybrid heterojunction for broadband photoresponse in visible to near infrared (IR) region under low reverse bias condition.

Origin of switching current transients in TIPS-pentacene based organic thin-film transistor with polymer dielectric

NASA Astrophysics Data System (ADS)

Singh, Subhash; Mohapatra, Y. N.

2017-06-01

We have investigated switch-on drain-source current transients in fully solution-processed thin film transistors based on 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS-pentacene) using cross-linked poly-4-vinylphenol as a dielectric. We show that the nature of the transient (increasing or decreasing) depends on both the temperature and the amplitude of the switching pulse at the gate. The isothermal transients are analyzed spectroscopically in a time domain to extract the degree of non-exponentiality and its possible origin in trap kinetics. We propose a phenomenological model in which the exchange of electrons between interfacial ions and traps controls the nature of the drain current transients dictated by the Fermi level position. The origin of interfacial ions is attributed to the essential fabrication step of UV-ozone treatment of the dielectric prior to semiconductor deposition.

Unified model for singlet fission within a non-conjugated covalent pentacene dimer

DOE PAGES

Basel, Bettina S.; Zirzlmeier, Johannes; Hetzer, Constantin; ...

2017-05-18

When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron–hole pairs, leading to a predicted B50% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state thatmore » precedes formation of the pentacene triplet excitons. In conclusion, using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.« less

Tuning charge transport in pentacene thin-film transistors using the strain-induced electron-phonon coupling modification

NASA Astrophysics Data System (ADS)

Lin, Yow-Jon; Chang, Hsing-Cheng; Liu, Day-Shan

2015-03-01

Tuning charge transport in the bottom-contact pentacene-based organic thin-film transistors (OTFTs) using a MoO x capping layer that serves to the electron-phonon coupling modification is reported. For OTFTs with a MoO x front gate, the enhanced field-effect carrier mobility is investigated. The time domain data confirm the electron-trapping model. To understand the origin of a mobility enhancement, an analysis of the temperature-dependent Hall-effect characteristics is presented. Similarly, the Hall-effect carrier mobility was dramatically increased by capping a MoO x layer on the pentacene front surface. However, the carrier concentration is not affected. The Hall-effect carrier mobility exhibits strong temperature dependence, indicating the dominance of tunneling (hopping) at low (high) temperatures. A mobility enhancement is considered to come from the electron-phonon coupling modification that results from the contribution of long-lifetime electron trapping.

Unified model for singlet fission within a non-conjugated covalent pentacene dimer

PubMed Central

Basel, Bettina S.; Zirzlmeier, Johannes; Hetzer, Constantin; Phelan, Brian T.; Krzyaniak, Matthew D.; Reddy, S. Rajagopala; Coto, Pedro B.; Horwitz, Noah E.; Young, Ryan M.; White, Fraser J.; Hampel, Frank; Clark, Timothy; Thoss, Michael; Tykwinski, Rik R.; Wasielewski, Michael R.; Guldi, Dirk M.

2017-01-01

When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron–hole pairs, leading to a predicted ∼50% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state that precedes formation of the pentacene triplet excitons. Using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures. PMID:28516916

Creating and optimizing interfaces for electric-field and photon-induced charge transfer.

PubMed

Park, Byoungnam; Whitham, Kevin; Cho, Jiung; Reichmanis, Elsa

2012-11-27

We create and optimize a structurally well-defined electron donor-acceptor planar heterojunction interface in which electric-field and/or photon-induced charge transfer occurs. Electric-field-induced charge transfer in the dark and exciton dissociation at a pentacene/PCBM interface were probed by in situ thickness-dependent threshold voltage shift measurements in field-effect transistor devices during the formation of the interface. Electric-field-induced charge transfer at the interface in the dark is correlated with development of the pentacene accumulation layer close to PCBM, that is, including interface area, and dielectric relaxation time in PCBM. Further, we demonstrate an in situ test structure that allows probing of both exciton diffusion length and charge transport properties, crucial for optimizing optoelectronic devices. Competition between the optical absorption length and the exciton diffusion length in pentacene governs exciton dissociation at the interface. Charge transfer mechanisms in the dark and under illumination are detailed.

Electronic Structure in Thin Film Organic Semiconductors

DTIC Science & Technology

2009-06-27

Peltekis, C. McGuinness, and A. Matsuura, J. Chem. Phys. 129, 224705, (2008) c) "The Local Electronic Structure of Tin Phthalocyanine studied by...interfaces in a Cu(100)-benzenethiolate- pentacene heterostructure", Phys. Rev. Lett. 100, 027601 (2008). 21. O.V. Molodtsova, M. Grobosch, M. Knupfer...1999). 37. N.J. Watkins, S. Zorba, and Y. Gao, "Interface formation of pentacene on Al2O3", J. Appl. Phys. 96, 425 (2004). 38. K.V. Chauhan, I

Kelvin probe microscopic visualization of charge storage at polystyrene interfaces with pentacene and gold

NASA Astrophysics Data System (ADS)

Dawidczyk, T. J.; Johns, G. L.; Ozgun, R.; Alley, O.; Andreou, A. G.; Markovic, N.; Katz, H. E.

2012-02-01

Charge carriers trapped in polystyrene (PS) were investigated with Kelvin probe microscopy (KPM) and thermally stimulated discharge current (TSDC). Lateral heterojunctions of pentacene/PS were scanned using KPM, effectively observing polarization along a side view of a lateral nonvolatile organic field-effect transistor dielectric interface. TSDC was used to observe charge migration out of PS films and to estimate the trap energy level inside the PS, using the initial rise method.

Pentacene on Au(1 1 1), Ag(1 1 1) and Cu(1 1 1): From physisorption to chemisorption.

PubMed

Lu, Meng-Chao; Wang, Rong-Bin; Yang, Ao; Duhm, Steffen

2016-03-09

We measured the electronic and the molecular surface structure of pentacene deposited on the (1 1 1)-surfaces of coinage metals by means of ultraviolet photoelectron spectroscopy (UPS) and low-energy electron diffraction (LEED). Pentacene is almost flat-lying in monolayers on all three substrates and highly ordered on Au(1 1 1) and on Cu(1 1 1). On Ag(1 1 1), however, weak chemisorption leads to almost disordered monolayers, both, at room temperature and at 78 K. On Cu(1 1 1) pentacene is strongly chemisorbed and the lowest unoccupied molecular orbital becomes observable in UPS by a charge transfer from the substrate. On Ag(1 1 1) and Cu(1 1 1) multilayers adopt a tilted orientation and a high degree of crystallinity. On Au(1 1 1), most likely, also in multilayers the molecular short and long axes are parallel to the substrate, leading to a distinctively different electronic structure than on Ag(1 1 1) and Cu(1 1 1). Overall, it could be demonstrated that the substrate not only determines the geometric and electronic characteristics of molecular monolayer films but also plays a crucial role for multilayer film growth.

Optimizing pentacene thin-film transistor performance: Temperature and surface condition induced layer growth modification.

PubMed

Lassnig, R; Hollerer, M; Striedinger, B; Fian, A; Stadlober, B; Winkler, A

2015-11-01

In this work we present in situ electrical and surface analytical, as well as ex situ atomic force microscopy (AFM) studies on temperature and surface condition induced pentacene layer growth modifications, leading to the selection of optimized deposition conditions and entailing performance improvements. We prepared p ++ -silicon/silicon dioxide bottom-gate, gold bottom-contact transistor samples and evaluated the pentacene layer growth for three different surface conditions (sputtered, sputtered + carbon and unsputtered + carbon) at sample temperatures during deposition of 200 K, 300 K and 350 K. The AFM investigations focused on the gold contacts, the silicon dioxide channel region and the highly critical transition area. Evaluations of coverage dependent saturation mobilities, threshold voltages and corresponding AFM analysis were able to confirm that the first 3-4 full monolayers contribute to the majority of charge transport within the channel region. At high temperatures and on sputtered surfaces uniform layer formation in the contact-channel transition area is limited by dewetting, leading to the formation of trenches and the partial development of double layer islands within the channel region instead of full wetting layers. By combining the advantages of an initial high temperature deposition (well-ordered islands in the channel) and a subsequent low temperature deposition (continuous film formation for low contact resistance) we were able to prepare very thin (8 ML) pentacene transistors of comparably high mobility.

Achievement of High-Response Organic Field-Effect Transistor NO₂ Sensor by Using the Synergistic Effect of ZnO/PMMA Hybrid Dielectric and CuPc/Pentacene Heterojunction.

PubMed

Han, Shijiao; Cheng, Jiang; Fan, Huidong; Yu, Junsheng; Li, Lu

2016-10-21

High-response organic field-effect transistor (OFET)-based NO₂ sensors were fabricated using the synergistic effect the synergistic effect of zinc oxide/poly(methyl methacrylate) (ZnO/PMMA) hybrid dielectric and CuPc/Pentacene heterojunction. Compared with the OFET sensors without synergistic effect, the fabricated OFET sensors showed a remarkable shift of saturation current, field-effect mobility and threshold voltage when exposed to various concentrations of NO₂ analyte. Moreover, after being stored in atmosphere for 30 days, the variation of saturation current increased more than 10 folds at 0.5 ppm NO₂. By analyzing the electrical characteristics, and the morphologies of organic semiconductor films of the OFET-based sensors, the performance enhancement was ascribed to the synergistic effect of the dielectric and organic semiconductor. The ZnO nanoparticles on PMMA dielectric surface decreased the grain size of pentacene formed on hybrid dielectric, facilitating the diffusion of CuPc molecules into the grain boundary of pentacene and the approach towards the conducting channel of OFET. Hence, NO₂ molecules could interact with CuPc and ZnO nanoparticles at the interface of dielectric and organic semiconductor. Our results provided a promising strategy for the design of high performance OFET-based NO₂ sensors in future electronic nose and environment monitoring.

Achievement of High-Response Organic Field-Effect Transistor NO2 Sensor by Using the Synergistic Effect of ZnO/PMMA Hybrid Dielectric and CuPc/Pentacene Heterojunction

PubMed Central

Han, Shijiao; Cheng, Jiang; Fan, Huidong; Yu, Junsheng; Li, Lu

2016-01-01

High-response organic field-effect transistor (OFET)-based NO2 sensors were fabricated using the synergistic effect the synergistic effect of zinc oxide/poly(methyl methacrylate) (ZnO/PMMA) hybrid dielectric and CuPc/Pentacene heterojunction. Compared with the OFET sensors without synergistic effect, the fabricated OFET sensors showed a remarkable shift of saturation current, field-effect mobility and threshold voltage when exposed to various concentrations of NO2 analyte. Moreover, after being stored in atmosphere for 30 days, the variation of saturation current increased more than 10 folds at 0.5 ppm NO2. By analyzing the electrical characteristics, and the morphologies of organic semiconductor films of the OFET-based sensors, the performance enhancement was ascribed to the synergistic effect of the dielectric and organic semiconductor. The ZnO nanoparticles on PMMA dielectric surface decreased the grain size of pentacene formed on hybrid dielectric, facilitating the diffusion of CuPc molecules into the grain boundary of pentacene and the approach towards the conducting channel of OFET. Hence, NO2 molecules could interact with CuPc and ZnO nanoparticles at the interface of dielectric and organic semiconductor. Our results provided a promising strategy for the design of high performance OFET-based NO2 sensors in future electronic nose and environment monitoring. PMID:27775653

Impact of pentacene film thickness on the photoresponse spectra: Determination of the photocarrier generation mechanism

NASA Astrophysics Data System (ADS)

Gorgolis, S.; Giannopoulou, A.; Anastassopoulos, D.; Kounavis, P.

2012-07-01

Photocurrent response, optical absorption, and x-ray diffraction (XRD) measurements in pentacene films grown on glass substrates are performed in order to obtain an insight into the mobile photocarriers generation mechanism. For film thickness of the order of 50 nm and lower, the photocurrent response spectra are found to follow the optical absorption spectra demonstrating the so-called symbatic response. Upon increasing the film thickness, the photoresponse demonstrates a transition to the so-called antibatic response, which is characterized by a maximum and minimum photocurrent for photon energies of minimum and maximum optical absorption, respectively. The experimental results are not in accordance with the model of important surface recombination rate. By taking into account the XRD patterns, the experimental photoresponse spectra can be reproduced by model simulations assuming efficient exciton dissociation at a narrow layer of the order of 20 nm near the pentacene-substrate interface. The simulated spectra are found sensitive to the film thickness, the absolute optical absorption coefficient, and the diffusion exciton length. By comparing the experimental with the simulated spectra, it is deduced that the excitons, which are created by optical excitation in the spectral region of 1.7-2.2 eV, diffuse with a diffusion length of the order of 10-80 nm to the pentacene-substrate interface where efficiently dissociate into mobile charge carriers.

Optimizing pentacene thin-film transistor performance: Temperature and surface condition induced layer growth modification

PubMed Central

Lassnig, R.; Hollerer, M.; Striedinger, B.; Fian, A.; Stadlober, B.; Winkler, A.

2015-01-01

In this work we present in situ electrical and surface analytical, as well as ex situ atomic force microscopy (AFM) studies on temperature and surface condition induced pentacene layer growth modifications, leading to the selection of optimized deposition conditions and entailing performance improvements. We prepared p++-silicon/silicon dioxide bottom-gate, gold bottom-contact transistor samples and evaluated the pentacene layer growth for three different surface conditions (sputtered, sputtered + carbon and unsputtered + carbon) at sample temperatures during deposition of 200 K, 300 K and 350 K. The AFM investigations focused on the gold contacts, the silicon dioxide channel region and the highly critical transition area. Evaluations of coverage dependent saturation mobilities, threshold voltages and corresponding AFM analysis were able to confirm that the first 3–4 full monolayers contribute to the majority of charge transport within the channel region. At high temperatures and on sputtered surfaces uniform layer formation in the contact–channel transition area is limited by dewetting, leading to the formation of trenches and the partial development of double layer islands within the channel region instead of full wetting layers. By combining the advantages of an initial high temperature deposition (well-ordered islands in the channel) and a subsequent low temperature deposition (continuous film formation for low contact resistance) we were able to prepare very thin (8 ML) pentacene transistors of comparably high mobility. PMID:26543442

Trap densities and transport properties of pentacene metal-oxide-semiconductor transistors: II—Numerical modeling of dc characteristics

NASA Astrophysics Data System (ADS)

Basile, A. F.; Kyndiah, A.; Biscarini, F.; Fraboni, B.

2014-06-01

A numerical procedure to calculate the drain-current (ID) vs. gate-voltage (VG) characteristics from numerical solutions of the Poisson equation for organic Thin-Film Transistors (TFTs) is presented. Polaron transport is modeled as two-dimensional charge transport in a semiconductor having free-carrier density of states proportional to the density of molecules and traps with energy equal to the polaron-hopping barrier. The simulated ID-VG curves are proportional to the product of the density of free carriers, calculated as a function of VG, and the intrinsic mobility, assumed to be a constant independent of temperature. The presence of traps in the oxide was also taken into account in the model, which was applied to a TFT made with six monolayers of pentacene grown on an oxide substrate. The polaron-hopping barrier determines the temperature dependence of the simulated ID-VG curves, trapping in the oxide is responsible for current reduction at high bias and the slope of the characteristics near threshold is related to the metal-semiconductor work-function difference. The values of the model parameters yielding the best match between calculations and experiments are consistent with previous experimental results and theoretical predictions. Therefore, this model enables to extract both physical and technological properties of thin-film devices from the temperature-dependent dc characteristics.

Properties of Poly- and Oligopentacenes Synthesized from Modular Building Blocks

DOE PAGES

Kumarasamy, Elango; Sanders, Samuel N.; Pun, Andrew B.; ...

2016-02-09

Here, we describe a facile route to well-defined, solution-processable pentacene oligomers (2 to 7) and homopolymer using Suzuki–Miyaura cross-coupling reactions. This synthetic strategy leads to regioisomers, regiopure syn- and anti-trimers were also synthesized, revealing minimal changes in solution properties but significant changes in the solid state arising from differing levels of crystallinity. The materials were characterized by steady state absorption spectroscopy and cyclic voltammetry to study their electronic structure. The steady state absorption spectra exhibit a new high-energy transition in the oligomers, which intensifies as a function of oligomer length, thus increasing the range of absorption to include the entiremore » visible spectrum. Density functional theory calculations indicate that the new peak results directly from the oligomerization. Solid state UV–vis suggests that while the monomer is amorphous, bricklayer packing in the higher oligomers significantly alters the solid state absorption relative to solution. The effect of oligomerization on packing was corroborated by GIWAXS analysis, which revealed crystalline domains in the oligomers. These domains, which are most evident in anti-trimer, become more pronounced upon thermal annealing. Photodegradation studies revealed considerable stability enhancement of oligomers toward oxygen and cycloaddition reactions relative to monomer. The synthesis and characterization of the first higher oligomers and homopolymer of pentacene should pave the way to applications in singlet fission, organic field-effect transistors, and organic photovoltaics.« less

Nonlinear Transport in Organic Thin Film Transistors with Soluble Small Molecule Semiconductor.

PubMed

Kim, Hyeok; Song, Dong-Seok; Kwon, Jin-Hyuk; Jung, Ji-Hoon; Kim, Do-Kyung; Kim, SeonMin; Kang, In Man; Park, Jonghoo; Tae, Heung-Sik; Battaglini, Nicolas; Lang, Philippe; Horowitz, Gilles; Bae, Jin-Hyuk

2016-03-01

Nonlinear transport is intensively explained through Poole-Frenkel (PF) transport mechanism in organic thin film transistors with solution-processed small molecules, which is, 6,13-bis(triisopropylsilylethynyl) (TIPS) pentacene. We outline a detailed electrical study that identifies the source to drain field dependent mobility. Devices with diverse channel lengths enable the extensive exhibition of field dependent mobility due to thermal activation of carriers among traps.

Multiscale Simulation and Modeling of Multilayer Heteroepitactic Growth of C60 on Pentacene.

PubMed

Acevedo, Yaset M; Cantrell, Rebecca A; Berard, Philip G; Koch, Donald L; Clancy, Paulette

2016-03-29

We apply multiscale methods to describe the strained growth of multiple layers of C60 on a thin film of pentacene. We study this growth in the presence of a monolayer pentacene step to compare our simulations to recent experimental studies by Breuer and Witte of submonolayer growth in the presence of monolayer steps. The molecular-level details of this organic semiconductor interface have ramifications on the macroscale structural and electronic behavior of this system and allow us to describe several unexplained experimental observations for this system. The growth of a C60 thin film on a pentacene surface is complicated by the differing crystal habits of the two component species, leading to heteroepitactical growth. In order to probe this growth, we use three computational methods that offer different approaches to coarse-graining the system and differing degrees of computational efficiency. We present a new, efficient reaction-diffusion continuum model for 2D systems whose results compare well with mesoscale kinetic Monte Carlo (KMC) results for submonolayer growth. KMC extends our ability to simulate multiple layers but requires a library of predefined rates for event transitions. Coarse-grained molecular dynamics (CGMD) circumvents KMC's need for predefined lattices, allowing defects and grain boundaries to provide a more realistic thin film morphology. For multilayer growth, in this particularly suitable candidate for coarse-graining, CGMD is a preferable approach to KMC. Combining the results from these three methods, we show that the lattice strain induced by heteroepitactical growth promotes 3D growth and the creation of defects in the first monolayer. The CGMD results are consistent with experimental results on the same system by Conrad et al. and by Breuer and Witte in which C60 aggregates change from a 2D structure at low temperature to 3D clusters along the pentacene step edges at higher temperatures.

Absence of Intramolecular Singlet Fission in Pentacene-Perylenediimide Heterodimers: The Role of Charge Transfer State.

PubMed

Wang, Long; Wu, Yishi; Chen, Jianwei; Wang, Lanfen; Liu, Yanping; Yu, Zhenyi; Yao, Jiannian; Fu, Hongbing

2017-11-16

A new class of donor-acceptor heterodimers based on two singlet fission (SF)-active chromophores, i.e., pentacene (Pc) and perylenediimide (PDI), was developed to investigate the role of charge transfer (CT) state on the excitonic dynamics. The CT state is efficiently generated upon photoexcitation. However, the resulting CT state decays to different energy states depending on the energy levels of the CT state. It undergoes extremely rapid deactivation to the ground state in polar CH 2 Cl 2 , whereas it undergoes transformation to a Pc triplet in nonpolar toluene. The efficient triplet generation in toluene is not due to SF but CT-mediated intersystem crossing. In light of the energy landscape, it is suggested that the deep energy level of the CT state relative to that of the triplet pair state makes the CT state actually serve as a trap state that cannot undergoes an intramolecular singlet fission process. These results provide guidance for the design of SF materials and highlight the requisite for more widely applicable design principles.

Optical second harmonic generation phase measurement at interfaces of some organic layers with indium tin oxide

NASA Astrophysics Data System (ADS)

Ngah Demon, Siti Zulaikha; Miyauchi, Yoshihiro; Mizutani, Goro; Matsushima, Toshinori; Murata, Hideyuki

2014-08-01

We observed phase shift in optical second harmonic generation (SHG) from interfaces of indium tin oxide (ITO)/copper phthalocyanine (CuPc) and ITO/pentacene. Phase correction due to Fresnel factors of the sample was taken into account. The phase of SHG electric field at the ITO/pentacene interface, ϕinterface with respect to the phase of SHG of bare substrate ITO was 160°, while the interface of ITO/CuPc had a phase of 140°.

Microstructural study of the polymorphic transformation in pentacene thin films.

PubMed

Murakami, Yosuke; Tomiya, Shigetaka; Koshitani, Naoki; Kudo, Yoshihiro; Satori, Kotaro; Itabashi, Masao; Kobayashi, Norihito; Nomoto, Kazumasa

2009-10-02

We have observed, by high-resolution cross-sectional transmission electron microscopy, the first direct evidence of polymorphic transformation in pentacene thin films deposited on silicon oxide substrates. Polymorphic transformation from the thin-film phase to the bulk phase occurred preferentially near polycrystalline grain boundaries, which exhibit concave surfaces. This process is thought to be driven by compressive stress caused by the grain boundaries. In addition to this stress, lattice mismatch between the two phases also results in structural defect formation.

First International Conference on Organic Nonlinear Optics. Section B: Nonlinear Optics, Principles, Materials, Phenomena, and Devices.

DTIC Science & Technology

1994-01-01

kET/T1T 2 ) (solid lines). clusters of guest molecules with local concentrations exceeding the average value of about 1 pentacene /(50 ,A) in the highest...that the transport topology of singlet excitation energy is determined by the local distribu- tions of pentacene guests in the crystal. A singlet...Pullman, USA S. Miyata (co-chair), Tokyo University of Technology and Agriculture, Tokyo, Japan Local Organizing Committee F. Charra (secretary) P.-A

Holographic Methods for the Investigation of Photophysical Properties.

DTIC Science & Technology

1983-04-22

terphenyl doped with 10- 3 mol/mol of pentacene . Obtaining k from decay curves as in * A -Fig. 14a and plotting k as a function of 02 (see Fig. 14b...translation diffusion of molecules in liquid solvents can be used to probe solute conformations, solvent-solute interactions and local solvent structure...eiion of 1.7omoAr WauW by TrArWAOn GFarinP So far, local heating by the absorption of the two interfering light pulses has not been taken into

One-dimensional self-confinement promotes polymorph selection in large-area organic semiconductor thin films.

PubMed

Giri, Gaurav; Li, Ruipeng; Smilgies, Detlef-M; Li, Er Qiang; Diao, Ying; Lenn, Kristina M; Chiu, Melanie; Lin, Debora W; Allen, Ranulfo; Reinspach, Julia; Mannsfeld, Stefan C B; Thoroddsen, Sigurdur T; Clancy, Paulette; Bao, Zhenan; Amassian, Aram

2014-04-16

A crystal's structure has significant impact on its resulting biological, physical, optical and electronic properties. In organic electronics, 6,13(bis-triisopropylsilylethynyl)pentacene (TIPS-pentacene), a small-molecule organic semiconductor, adopts metastable polymorphs possessing significantly faster charge transport than the equilibrium crystal when deposited using the solution-shearing method. Here, we use a combination of high-speed polarized optical microscopy, in situ microbeam grazing incidence wide-angle X-ray-scattering and molecular simulations to understand the mechanism behind formation of metastable TIPS-pentacene polymorphs. We observe that thin-film crystallization occurs first at the air-solution interface, and nanoscale vertical spatial confinement of the solution results in formation of metastable polymorphs, a one-dimensional and large-area analogy to crystallization of polymorphs in nanoporous matrices. We demonstrate that metastable polymorphism can be tuned with unprecedented control and produced over large areas by either varying physical confinement conditions or by tuning energetic conditions during crystallization through use of solvent molecules of various sizes.

Long-Lived Correlated Triplet Pairs in a π-Stacked Crystalline Pentacene Derivative.

PubMed

Folie, Brendan D; Haber, Jonah B; Refaely-Abramson, Sivan; Neaton, Jeffrey B; Ginsberg, Naomi S

2018-02-14

Singlet fission is the spin-conserving process by which a singlet exciton splits into two triplet excitons. Singlet fission occurs via a correlated triplet pair intermediate, but direct evidence of this state has been scant, and in films of TIPS-pentacene, a small molecule organic semiconductor, even the rate of fission has been unclear. We use polarization-resolved transient absorption microscopy on individual crystalline domains of TIPS-pentacene to establish the fission rate and demonstrate that the initially created triplets remain bound for a surprisingly long time, hundreds of picoseconds, before separating. Furthermore, using a broadband probe, we show that it is possible to determine absorbance spectra of individual excited species in a crystalline solid. We find that triplet interactions perturb the absorbance, and provide evidence that triplet interaction and binding could be caused by the π-stacked geometry. Elucidating the relationship between the lattice structure and the electronic structure and dynamics has important implications for the creation of photovoltaic devices that aim to boost efficiency via singlet fission.

High-performance pentacene OTFT by incorporating Ti in LaON gate dielectric

NASA Astrophysics Data System (ADS)

Ma, Y. X.; Han, C. Y.; Tang, W. M.; Lai, P. T.

2017-07-01

Pentacene organic thin-film transistors (OTFT) using high-k LaTiON gate dielectric with different Ti contents are investigated. The LaxTi(1-x)ON films (with x = 1, 0.87, 0.76, and 0.67) are deposited by reactive sputtering followed by an annealing in N2 at 200 °C. The OTFT with La0.87Ti0.13ON can achieve a high carrier mobility of 2.6 cm2/V.s, a small threshold voltage of -1.5 V, a small sub-threshold swing of 0.07 V/dec, and a small hysteresis of 0.17 V. AFM and X-ray photoelectron spectroscopy reveal that Ti can suppress the hygroscopicity of La oxide to achieve a smoother dielectric surface, which can result in larger pentacene grains and thus higher carrier mobility. All the devices show a clockwise hysteresis because both the LaOH formation and Ti incorporation can generate acceptor-like traps in the gate dielectric.

Determination of diffusion coefficient in disordered organic semiconductors

NASA Astrophysics Data System (ADS)

Rani, Varsha; Sharma, Akanksha; Ghosh, Subhasis

2016-05-01

Charge carrier transport in organic semiconductors is dominated by positional and energetic disorder in Gaussian density of states (GDOS) and is characterized by hopping through localized states. Due to the immobilization of charge carriers in these localized states, significant non-uniform carrier distribution exists, resulting diffusive transport. A simple, nevertheless powerful technique to determine diffusion coefficient D in disordered organic semiconductors has been presented. Diffusion coefficients of charge carriers in two technologically important organic molecular semiconductors, Pentacene and copper phthalocyanine (CuPc) have been measured from current-voltage (J-V) characteristics of Al/Pentacene/Au and Al/CuPc/Au based Schottky diodes. Ideality factor g and carrier mobility μ have been calculated from the exponential and space charge limited region respectively of J-V characteristics. Classical Einstein relation is not valid in organic semiconductors due to energetic disorders in DOS. Using generalized Einstein relation, diffusion coefficients have been obtained to be 1.31×10-6 and 1.73×10-7 cm2/s for Pentacene and CuPc respectively.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tayebjee, Murad J. Y.; Sanders, Samuel N.; Kumarasamy, Elango

Singlet fission, in which two triplet excitons are generated from a single absorbed photon, is a key third-generation solar cell concept. Conservation of angular momentum requires that singlet fission populates correlated multiexciton states, which can subsequently dissociate to generate free triplets. However, little is known about electronic and spin correlations in these systems since, due to its typically short lifetime, the multiexciton state is challenging to isolate and study. Here, we use bridged pentacene dimers, which undergo intramolecular singlet fission while isolated in solution and in solid matrices, as a unimolecular model system that can trap long-lived multiexciton states. Wemore » also combine transient absorption and time-resolved electron spin resonance spectroscopies to show that spin correlations in the multiexciton state persist for hundreds of nanoseconds. Furthermore, we confirm long-standing predictions that singlet fission produces triplet pair states of quintet character. Finally, we compare two different pentacene–bridge–pentacene chromophores, systematically tuning the coupling between the pentacenes to understand how differences in molecular structure affect the population and dissociation of multiexciton quintet states.« less

Semiconducting molecular crystals: Bulk in-gap states modified by structural and chemical defects

NASA Astrophysics Data System (ADS)

Haas, S.; Krellner, C.; Goldmann, C.; Pernstich, K. P.; Gundlach, D. J.; Batlogg, B.

2007-03-01

Charge transport in organic molecular crystals is strongly influenced by the density of localized in-gap states (traps). Thus, a profound knowledge of the defect states' origin is essential. Temperature-dependent space-charge limited current (TD-SCLC) spectroscopy was used as a powerful tool to quantitatively study the density of states (DOS) in high-quality rubrene and pentacene single crystals. In particular, changes of the DOS due to intentionally induced chemical and structural defects were monitored. For instance, the controlled exposure of pentacene and rubrene to x-ray radiation results in a broad over-all increase of the DOS. Namely, the ionizing radiation induces a variety of both chemical and structural defects. On the other hand, exposure of rubrene to UV-excited oxygen is reflected in a sharp peak in the DOS, whereas in a similar experiment with pentacene oxygen acts as a dopant, and possible defects are metastable on the time-scale of the measurement, thus leaving the extracted DOS virtually unchanged.

Sub-micron phase coexistence in small-molecule organic thin films revealed by infrared nano-imaging

PubMed Central

Westermeier, Christian; Cernescu, Adrian; Amarie, Sergiu; Liewald, Clemens; Keilmann, Fritz; Nickel, Bert

2014-01-01

Controlling the domain size and degree of crystallization in organic films is highly important for electronic applications such as organic photovoltaics, but suitable nanoscale mapping is very difficult. Here we apply infrared-spectroscopic nano-imaging to directly determine the local crystallinity of organic thin films with 20-nm resolution. We find that state-of-the-art pentacene films (grown on SiO2 at elevated temperature) are structurally not homogeneous but exhibit two interpenetrating phases at sub-micrometre scale, documented by a shifted vibrational resonance. We observe bulk-phase nucleation of distinct ellipsoidal shape within the dominant pentacene thin-film phase and also further growth during storage. A faint topographical contrast as well as X-ray analysis corroborates our interpretation. As bulk-phase nucleation obstructs carrier percolation paths within the thin-film phase, hitherto uncontrolled structural inhomogeneity might have caused conflicting reports about pentacene carrier mobility. Infrared-spectroscopic nano-imaging of nanoscale polymorphism should have many applications ranging from organic nanocomposites to geologic minerals. PMID:24916130

Charge carriers' trapping states in pentacene films studied by modulated photocurrent

NASA Astrophysics Data System (ADS)

Gorgolis, S.; Giannopoulou, A.; Kounavis, P.

2013-03-01

The modulated photocurrent (MPC) technique is employed to study the charge carriers' trapping states of pentacene films. The characteristics of the experimental MPC spectra were found to be compatible with trapping-detrapping process of holes in gap states in which their occupancy can be modified by the bias illumination. A demarcation energy level separating empty from partially occupied traps was deduced from the MPC spectra, which can be used to monitor bias-light induced changes in the quasi Fermi level. An exponential trap distribution from structural disorder and a deep metastable gaussian trap distribution from adsorbed environmental impurities were extracted by means of the MPC spectroscopy. An attempt to escape frequency of the order of 1010s-1 was deduced for the gap sates. The derived trap distributions agree with those found before by means of other techniques. The present results indicate that the MPC technique can be used as a valuable tool for pentacene films characterization since it can be also applied to field effect samples.

Effect of Vertical Annealing on the Nitrogen Dioxide Response of Organic Thin Film Transistors

PubMed Central

Hou, Sihui; Zhuang, Xinming; Yang, Zuchong

2018-01-01

Nitrogen dioxide (NO2) sensors based on organic thin-film transistors (OTFTs) were fabricated by conventional annealing (horizontal) and vertical annealing processes of organic semiconductor (OSC) films. The NO2 responsivity of OTFTs to 15 ppm of NO2 is 1408% under conditions of vertical annealing and only 72% when conventional annealing is applied. Moreover, gas sensors obtained by vertical annealing achieve a high sensing performance of 589% already at 1 ppm of NO2, while showing a preferential response to NO2 compared with SO2, NH3, CO, and H2S. To analyze the mechanism of performance improvement of OTFT gas sensors, the morphologies of 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS-pentacene) films were characterized by atomic force microscopy (AFM) in tapping mode. The results show that, in well-aligned TIPS-pentacene films, a large number of effective grain boundaries inside the conducting channel contribute to the enhancement of NO2 gas sensing performance. PMID:29596331

Infrared Spectroscopy of Matrix-Isolated Polycyclic Aromatic Hydrocarbon Cations. 3; The Polyacenes Anthracene, Tetracence, and Pentacene

NASA Technical Reports Server (NTRS)

Hudgins, D. M.; Allamandola, L. J.

1995-01-01

Gaseous, ionized polycyclic aromatic hydrocarbons (PAHS) are thought to be responsible for a very common family of interstellar infrared emission bands. Unfortunately, very little infrared spectroscopic data are available on ionized PAHS. Here we present the near- and mid-infrared spectra of the polyacene cations anthracene, tetracene, and pentacene. We also report the vibrational frequencies and relative intensities of the pentacene anion. The cation bands corresponding to the CC modes are typically about 10-20 times more intense than those of the CH out-of-plane bending vibrations. For the cations the CC stretching and CH in-plane bending modes give rise to bands which are an order of magnitude stronger than for the neutral species, and the CH out-of-plane bends produce bands which are 3-20 times weaker than in the neutral species. This behavior is similar to that found for most other PAH cations. The most intense PAH cation bands fall within the envelopes of the most intense interstellar features. The strongest absorptions in the polyacenes anthracene, tetracene, and pentacene tend to group around 1400/cm (between about 1340 and 1500/cm) and near 1180/cm, regions of only moderate interstellar emission. These very strong polyacene bands tend to fall in gaps in the spectra of the other PAH cations studied to date suggesting that while PAHs with polyacene structures may contribute to specific regions of the interstellar emission spectra, they are not dominant members of the interstellar PAH family.

Infrared Spectroscopy of Matrix-Isolated Polycyclic Aromatic Hydrocarbon Cations. 3. The Polyacenes Anthracene, Tetracene, and Pentacene

NASA Technical Reports Server (NTRS)

Hudgins, D. M.; Allamandola, L. J.

1995-01-01

Gaseous, ionized Polycyclic Aromatic Hydrocarbons (PAH's) are thought to be responsible for a very common family of interstellar infrared emission bands. Unfortunately, very little infrared spectroscopic data are available on ionized PAH's. Here we present the near- and mid-infrared spectra of the polyacene cations anthracene, tetracene, and pentacene. We also report the vibrational frequencies and relative intensities of the pentacene anion. The cation bands corresponding to the CC modes are typically about 10-20 times more intense than those of the CH out-of-plane bending vibrations. For the cations the CC stretching and CH in-plane bending modes give rise to bands which are an order of magnitude stronger than for the neutral species, and the CH out-of-plane bends produce bands which are 3-20 times weaker than in the neutral species. This behavior is similar to that found for most other PAH cations. The most intense PAH cation bands fall within the envelopes of the most intense interstellar features. The strongest absorptions in the polyacenes anthracene, tetracene, and pentacene tend to group around 1400 / cm (between about 1340 and 1500 / cm) and near 1180 /cm, regions of only moderate interstellar emission. These very strong polyacene bands tend to fall in gaps in the spectra of the other PAH cations studied to date suggesting that while PAHs with polyacene structures may contribute to specific regions of the interstellar emission spectra, they are not dominant members of the interstellar PAH family.

Unusual Thermoelectric Behavior Indicating a Hopping to Bandlike Transport Transition in Pentacene

NASA Astrophysics Data System (ADS)

Germs, W. Chr.; Guo, K.; Janssen, R. A. J.; Kemerink, M.

2012-07-01

An unusual increase in the Seebeck coefficient with increasing charge carrier density is observed in pentacene thin film transistors. This behavior is interpreted as being due to a transition from hopping transport in static localized states to bandlike transport, occurring at temperatures below ˜250K. Such a transition can be expected for organic materials in which both static energetic disorder and dynamic positional disorder are important. While clearly visible in the temperature and density dependent Seebeck coefficient, the transition hardly shows up in the charge carrier mobility.

Organic Based Flexible Transistors and Electronic Device

DTIC Science & Technology

2005-05-01

reactive groups that can act as charge carrier traps . 0.0 0.0 V1 ......3..... ... 10 " -.....-." . ;Z 0. - - -1,6 -V* /7VIDS -04O -2.5 10 -1.0 -0.8...of 2.5 kHz in vacuum with pentacene and DHFCO-4T with 7.5 ptm channel length devices. "* Ring oscillator frequencies of 10 kHz in air with pentacene ...similar herringbone packing in DFCO-4T (c) and DPCO-4T (d), respectively, viewed along the long crystallographic axis. Table 1. Charge carrier mobilities (A

Theory of Charge Transport in Organic Crystals: Lessons from the Past and Prospects for the Future

NASA Astrophysics Data System (ADS)

Kenkre, V. M.

2002-03-01

Interest in fundamental issues regarding charge transport in organic materials shifted in the early 80's from the field of crystals to the field of disordered systems after polaron theories[1,2] were successfully applied[2] to what was suspected to be a mobility transition in naphthalene[3]. Recent experiments on pentacene[4] have been responsible for a reversal of the shift: there is now a revival of interest in crystals particularly in basic questions regarding electron-phonon interactions, polaron formation, the nature of charge carriers, and the issue of band versus hopping transport. High magnitudes of the new mobilities appear to imply large free carrier bandwidths which have led some to conjecture that band (rather than hopping) transport is characteristic of pentacene[5]. And yet, pentacene experiments show an unmistakable rise in the mobility at higher temperature, a rise that seems to signal polaronic behavior. Added to this fascinating mélange of facts are clear velocity saturation effects[6] observed in pentacene[4] along with some cavalier interpretation attempts of those non-Ohmic effects. The purpose of the talk is to attempt to address basic issues raised by these observations. 1. R. Silbey and R. W. Munn, J. Chem. Phys. 72, 2763 (1980). 2. V. M. Kenkre, John D. Andersen, D.H. Dunlap, and C.B. Duke, Phys. Rev. Lett. 62, 1165 (1989); see also M. Pope and C. E. Swenberg, Electronic Processes in Organic Crystals and Polymers, 2nd ed. (Oxford Univ Press, New Yourk 1999), p. 968. 3. L. B. Schein, C. B. Duke, and A.R. McGhie, Phys. Rev. Lett. 40, 197 (1978); C. B. Duke and L. B. Schein, Physics Today 33, 42 (1980). 4. J. H. Schoen, C. Kloc, and B. Batlogg, Phys. Rev. Lett. 86, 3843 (2001); Phys. Rev. B63, 245201 (2001). 5. Note, however, a recent demonstration against bare band descriptions in pentacene provided by J. D. Andersen, L. Giuggioli, and V. M. Kenkre, Phys. Rev. B, submitted. 6. V. M. Kenkre and P. E. Parris, Phys. Rev. B, submitted; P. E. Parris, M. Kús and V. M. Kenkre, Phys. Lett. A 289, 188 (2001).

External quantum efficiency exceeding 100% in a singlet-exciton-fission-based solar cell

NASA Astrophysics Data System (ADS)

Baldo, Marc

2013-03-01

Singlet exciton fission can be used to split a molecular excited state in two. In solar cells, it promises to double the photocurrent from high energy photons, thereby breaking the single junction efficiency limit. We demonstrate organic solar cells that exploit singlet exciton fission in pentacene to generate more than one electron per incident photon in the visible spectrum. Using a fullerene acceptor, a poly(3-hexylthiophene) exciton confinement layer, and a conventional optical trapping scheme, the peak external quantum efficiency is (109 +/-1)% at λ = 670 nm for a 15-nm-thick pentacene film. The corresponding internal quantum efficiency is (160 +/-10)%. Independent confirmation of the high internal efficiency is obtained by analysis of the magnetic field effect on photocurrent, which determines that the triplet yield approaches 200% for pentacene films thicker than 5 nm. To our knowledge, this is the first solar cell to generate quantum efficiencies above 100% in the visible spectrum. Alternative multiple exciton generation approaches have been demonstrated previously in the ultraviolet, where there is relatively little sunlight. Singlet exciton fission differs from these other mechanisms because spin conservation disallows the usual dominant loss process: a thermal relaxation of the high-energy exciton into a single low-energy exciton. Consequently, pentacene is efficient in the visible spectrum at λ = 670 nm because only the collapse of the singlet exciton into twotriplets is spin-allowed. Supported as part of the Center for Excitonics, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award Number DE-SC0001088.

Imaging prototypical aromatic molecules on insulating surfaces: a review

NASA Astrophysics Data System (ADS)

Hoffmann-Vogel, R.

2018-01-01

Insulating substrates allow for in-plane contacted molecular electronics devices where the molecule is in contact with the insulator. For the development of such devices it is important to understand the interaction of molecules with insulating surfaces. As substrates, ionic crystals such as KBr, KCl, NaCl and CaF2 are discussed. The surface energies of these substrates are small and as a consequence intrinsic properties of the molecules, such as molecule–molecule interaction, become more important relative to interactions with the substrates. As prototypical molecules, three variants of graphene-related molecules are used, pentacene, C60 and PTCDA. Pentacene is a good candidate for molecular electronics applications due to its high charge carrier mobility. It shows mainly an upright standing growth mode and the morphology of the islands is strongly influenced by dewetting. A new second flat-lying phase of the molecule has been observed. Studying the local work function using the Kelvin method reveals details such as line defects in the center of islands. The local work function differences between the upright-standing and flat-lying phase can only be explained by charge transfer that is unusual on ionic crystalline surfaces. C60 nucleation and growth is explained by loosely bound molecules at kink sites as nucleation sites. The stability of C60 islands as a function of magic numbers is investigated. Peculiar island shapes are obtained from unusual dewetting processes already at work during growth, where molecules ‘climb’ to the second molecular layer. PTCDA is a prototypical semiconducting molecule with strong quadrupole moment. It grows in the form of elongated islands where the top and the facets can be molecularly resolved. In this way the precise molecular arrangement in the islands is revealed.

Quintet multiexciton dynamics in singlet fission

DOE PAGES

Tayebjee, Murad J. Y.; Sanders, Samuel N.; Kumarasamy, Elango; ...

2016-10-17

Singlet fission, in which two triplet excitons are generated from a single absorbed photon, is a key third-generation solar cell concept. Conservation of angular momentum requires that singlet fission populates correlated multiexciton states, which can subsequently dissociate to generate free triplets. However, little is known about electronic and spin correlations in these systems since, due to its typically short lifetime, the multiexciton state is challenging to isolate and study. Here, we use bridged pentacene dimers, which undergo intramolecular singlet fission while isolated in solution and in solid matrices, as a unimolecular model system that can trap long-lived multiexciton states. Wemore » also combine transient absorption and time-resolved electron spin resonance spectroscopies to show that spin correlations in the multiexciton state persist for hundreds of nanoseconds. Furthermore, we confirm long-standing predictions that singlet fission produces triplet pair states of quintet character. Finally, we compare two different pentacene–bridge–pentacene chromophores, systematically tuning the coupling between the pentacenes to understand how differences in molecular structure affect the population and dissociation of multiexciton quintet states.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lee, Juhee; Lee, Sungpyo; Lee, Moo Hyung

Quasi-unipolar non-volatile organic transistor memory (NOTM) can combine the best characteristics of conventional unipolar and ambipolar NOTMs and, as a result, exhibit improved device performance. Unipolar NOTMs typically exhibit a large signal ratio between the programmed and erased current signals but also require a large voltage to program and erase the memory cells. Meanwhile, an ambipolar NOTM can be programmed and erased at lower voltages, but the resulting signal ratio is small. By embedding a discontinuous n-type fullerene layer within a p-type pentacene film, quasi-unipolar NOTMs are fabricated, of which the signal storage utilizes both electrons and holes while themore » electrical signal relies on only hole conduction. These devices exhibit superior memory performance relative to both pristine unipolar pentacene devices and ambipolar fullerene/pentacene bilayer devices. The quasi-unipolar NOTM exhibited a larger signal ratio between the programmed and erased states while also reducing the voltage required to program and erase a memory cell. This simple approach should be readily applicable for various combinations of advanced organic semiconductors that have been recently developed and thereby should make a significant impact on organic memory research.« less

Exciton self-trapping and Stark effect in the optical response of pentacene crystals from first principles

NASA Astrophysics Data System (ADS)

Strubbe, David A.; Sharifzadeh, Sahar; Neaton, Jeffrey B.; Louie, Steven G.

2012-02-01

Pentacene is a prototypical organic semiconductor with optoelectronic and photovoltaic applications. It is known that the lowest-energy singlet excitation has a Stokes shift between absorption and emission of about 0.14 eV, but the deformation associated with this self-trapped exciton remains unknown. We begin with a calculation of the optical properties via the first-principles GW/Bethe-Salpeter (BSE) theory [ML Tiago, JE Northrup, and SG Louie, Phys. Rev. B 67, 115212 (2003); S Sharifzadeh, A Biller, L Kronik, and JB Neaton, arXiv:1110.4928 (2011)]. We then study the self-trapping phenomenon via our reformulation of the Bethe-Salpeter excited-state forces approximation of Ismail-Beigi and Louie [Phys. Rev. Lett. 90, 076401 (2003)], which can describe the structural relaxation after optical excitation. Whether excitons in pentacene have charge-transfer character has been controversial in electro-absorption experiments. We use the same BSE analytic derivatives approach to calculate the changes in excitation energies due to an applied electric field to understand this experimental controversy.

Effects of Gold Nanoparticles on Pentacene Organic Field-Effect Transistors

NASA Astrophysics Data System (ADS)

Lee, Keanchuan; Weis, Martin; Ou-Yang, Wei; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2011-04-01

The effect of gold nanoparticles (NPs) on pentacene organic field-effect transistors (OFETs) was being investigated by both DC and AC methods, which are current-voltage (I-V) measurements in steady-state and impedance spectroscopy (IS) respectively. Here poly(vinyl alcohol) (PVA) and PVA blended with Au NPs as composite are spin-coated on SiO2 as gate-insulator for top-contact pentacene OFET. The characteristics of the device were being investigated based on the contact resistance, trapped charges, effective mobility and threshold voltage based on transfer characteristics of OFET. Results revealed that OFET with NPs exhibited larger hysteresis and higher contact resistance at high voltage region. IS measurements were performed and the fitting of results by the Maxwell-Wagner equivalent circuit showed that for device with NPs a series of capacitance and resistance which represents trapping must be introduced in order to have agreeable fitting. The fitting had helped to clarify the reason behind the higher contact resistance and bigger hysteresis which was mainly caused by the space charge field formed by the traps when Au NPs were introduced into the device.

Microstructural control over soluble pentacene deposited by capillary pen printing for organic electronics.

PubMed

Lee, Wi Hyoung; Min, Honggi; Park, Namwoo; Lee, Junghwi; Seo, Eunsuk; Kang, Boseok; Cho, Kilwon; Lee, Hwa Sung

2013-08-28

Research into printing techniques has received special attention for the commercialization of cost-efficient organic electronics. Here, we have developed a capillary pen printing technique to realize a large-area pattern array of organic transistors and systematically investigated self-organization behavior of printed soluble organic semiconductor ink. The capillary pen-printed deposits of organic semiconductor, 6,13-bis(triisopropylsilylethynyl) pentacene (TIPS_PEN), was well-optimized in terms of morphological and microstructural properties by using ink with mixed solvents of chlorobenzene (CB) and 1,2-dichlorobenzene (DCB). Especially, a 1:1 solvent ratio results in the best transistor performances. This result is attributed to the unique evaporation characteristics of the TIPS_PEN deposits where fast evaporation of CB induces a morphological evolution at the initial printed position, and the remaining DCB with slow evaporation rate offers a favorable crystal evolution at the pinned position. Finally, a large-area transistor array was facilely fabricated by drawing organic electrodes and active layers with a versatile capillary pen. Our approach provides an efficient printing technique for fabricating large-area arrays of organic electronics and further suggests a methodology to enhance their performances by microstructural control of the printed organic semiconducting deposits.

Comparative study on degradation and trap density-of-states of p type and n type organic semiconductors

NASA Astrophysics Data System (ADS)

Shijeesh, M. R.; Vikas, L. S.; Jayaraj, M. K.; Puigdollers, J.

2014-10-01

The OTFTs with both p type and n type channel layers were fabricated using the inverted-staggered (top contact) structure by thermal vapour deposition on Si/SiO2 substrate. Pentacene and N,N'-Dioctyl- 3,4,9,10- perylenedicarboximide (PTCDI-C8) were used as channel layer for the fabrications of p type and n type OTFTs respectively. A comparative study on the degradation and density of states (DOS) of p type and n type organic semiconductors have been carried out. In order to compare the stability and degradation of pentacene and PTCDI-C8 OTFTs, the devices were exposed to air for 2 h before performing electrical measurements in air. The DOS measurements revealed that a level with defect density of 1020 cm-3 was formed only in PTCDI C8 layer on exposure to air. The oxygen adsorption into the PTCDI-C8 active layer can be attributed to the formation of this level at 0.15 eV above the LUMO level. The electrical charge transport is strongly affected by the oxygen traps and hence n type organic materials are less stable than p type organic materials.

Effect of UV/ozone treatment on polystyrene dielectric and its application on organic field-effect transistors

PubMed Central

2014-01-01

The influence of UV/ozone treatment on the property of polystyrene (PS) dielectric surface was investigated, and pentacene organic field-effect transistors (OFETs) based on the treated dielectric was fabricated. The dielectric and pentacene active layers were characterized by atomic force microscopy, X-ray photoelectron spectroscopy, and scanning electron microscopy. The results showed that, at short UVO exposure time (<10 s), the chemical composition of PS dielectric surface remained the same. While at long UVO exposure time (>60 s), new chemical groups, including alcohol/ether, carbonyl, and carboxyl/ester groups, were formed. By adjusting the UVO exposure time to 5 s, the hole mobility of the OFETs increased to 0.52 cm2/Vs, and the threshold voltage was positively shifted to -12 V. While the time of UVO treatment exceeded 30 s, the mobility started to shrink, and the off-current was enlarged. These results indicate that, as a simple surface treatment method, UVO treatment could quantitatively modulate the property of PS dielectric surface by controlling the exposure time, and thus, pioneered a new way to modulate the characteristics of organic electronic devices. PMID:25258603

Frenkel versus charge-transfer exciton dispersion in molecular crystals

NASA Astrophysics Data System (ADS)

Cudazzo, Pierluigi; Gatti, Matteo; Rubio, Angel; Sottile, Francesco

2013-11-01

By solving the many-body Bethe-Salpeter equation at finite momentum transfer, we characterize the exciton dispersion in two prototypical molecular crystals, picene and pentacene, in which localized Frenkel excitons compete with delocalized charge-transfer excitons. We explain the exciton dispersion on the basis of the interplay between electron and hole hopping and electron-hole exchange interaction, unraveling a simple microscopic description to distinguish Frenkel and charge-transfer excitons. This analysis is general and can be applied to other systems in which the electron wave functions are strongly localized, as in strongly correlated insulators.

Hall-Effect Measurements Probing the Degree of Charge-Carrier Delocalization in Solution-Processed Crystalline Molecular Semiconductors

NASA Astrophysics Data System (ADS)

Chang, Jui-Fen; Sakanoue, Tomo; Olivier, Yoann; Uemura, Takafumi; Dufourg-Madec, Marie-Beatrice; Yeates, Stephen G.; Cornil, Jérôme; Takeya, Jun; Troisi, Alessandro; Sirringhaus, Henning

2011-08-01

Intramolecular structure and intermolecular packing in crystalline molecular semiconductors should have profound effects on the charge-carrier wave function, but simple drift mobility measurements are not very sensitive to this. Here we show that differences in the Hall resistance of two soluble pentacene derivatives can be explained with different degrees of carrier delocalization being limited by thermal lattice fluctuations. A combination of Hall measurements, optical spectroscopy, and theoretical simulations provides a powerful probe of structure-property relationships at a molecular level.

Large Spatially Resolved Rectification in a Donor–Acceptor Molecular Heterojunction

DOE PAGES

Smerdon, Joseph A.; Giebink, Noel C.; Guisinger, Nathan P.; ...

2016-03-10

Here, we demonstrate that rectification ratios (RR) of ≳250 (≳1000) at biases of 0.5 V (1.2 V) are achievable at the two-molecule limit for donor–acceptor bilayers of pentacene on C 60 on Cu using scanning tunneling spectroscopy and microscopy. Using first-principles calculations, we show that the system behaves as a molecular Schottky diode with a tunneling transport mechanism from semiconducting pentacene to Cu- hybridized metallic C 60. Low-bias RRs vary by two orders-of-magnitude at the edge of these molecular heterojunctions due to increased Stark shifts and confinement effects.

Linear acene derivatives - New routes to pentacene and naphthacene and the first synthesis of a triptycene with two anthracene moieties

NASA Technical Reports Server (NTRS)

Luo, Jihmei; Hart, Harold

1987-01-01

The cycloaddition of o-xylylene to arene 1,4-endoxides was used to construct linear arene derivatives. An analogous sequence but with naphthalene 1,4-endoxides gave naphthacenes. Dehydration of the di adducts from 4 and anthracene 1,4:5,8-diendoxides gave a mixture of 5,9,14,18- and 5,8,15,18-tetrahydroheptacenes 3 and 9. The previously unknown triptycene 2 was synthesized from 5,14-dihydropentacene, an intermediate in the new pentacene synthesis, in three steps and 29 percent overall yield.

Initiation of Collapsing Pentacene Crystal by Au

NASA Astrophysics Data System (ADS)

Ihm, Kyuwook; Lee, Kyoung-Jae; Chung, Sukmin; Kang, Tai-Hee

2011-12-01

Metal contacts with gold on organics are an essential factor in organic electronics. The unveiled key challenge is to probe dynamic details of the microscopic evolution of the organic crystal when the atomic Au is introduced. Here, we show how the collapse of the pentacene crystal is initiated even by a few Au atoms. Our photoemission and x-ray absorption results indicate that the gentle decoupling of intra and inter-molecular π-π interactions causes the localization of the lowest unoccupied molecular orbital as well as the removal of cohesive forces between molecules, leading to the subsequent crystal collapse.

Early stages of collapsing pentacene crystal by Au

NASA Astrophysics Data System (ADS)

Ihm, Kyuwook; Chung, Sukmin; Kang, Tai-Hee; Cheong, Sang-Wook

2008-10-01

The characteristic feature of metal contacts with gold on organics is deterioration of the organic crystals during the contact formation. The unveiled key challenge is to probe dynamic details of the microscopic evolution of the organic crystal when the atomic Au is introduced. Here, we report how the collapse of the pentacene crystal is initiated even by a few Au atoms. Our results indicate that the gentle decoupling of intra and intermolecular π-π interactions causes the localization of the lowest unoccupied molecular orbital as well as the removal of cohesive forces between molecules, leading to the subsequent crystal collapse.

Gate bias stress in pentacene field-effect-transistors: Charge trapping in the dielectric or semiconductor

NASA Astrophysics Data System (ADS)

Häusermann, R.; Batlogg, B.

2011-08-01

Gate bias stress instability in organic field-effect transistors (OFETs) is a major conceptual and device issue. This effect manifests itself by an undesirable shift of the transfer characteristics and is associated with long term charge trapping. We study the role of the dielectric and the semiconductor separately by producing OFETs with the same semiconductor (pentacene) combined with different dielectrics (SiO2 and Cytop). We show that it is possible to fabricate devices which are immune to gate bias stress. For other material combinations, charge trapping occurs in the semiconductor alone or in the dielectric.

Time-resolved electric force microscopy of charge trapping in polycrystalline pentacene.

PubMed

Jaquith, Michael; Muller, Erik M; Marohn, John A

2007-07-12

Here we introduce time-resolved electric force microscopy measurements to directly and locally probe the kinetics of charge trap formation in a polycrystalline pentacene thin-film transistor. We find that the trapping rate depends strongly on the initial concentration of free holes and that trapped charge is highly localized. The observed dependence of trapping rate on the hole chemical potential suggests that the trapping process should not be viewed as a filling of midgap energy levels, but instead as a process in which the very creation of trapped states requires the presence of free holes.

A density-functional-theory study of biradicals from benzene to hexacene

NASA Astrophysics Data System (ADS)

Kim, Hyun-Jung; Wang, Xingyong; Ma, Jing; Cho, Jun-Hyung

2011-11-01

The singlet-triplet energy gap of biradicals created in benzene and polyacenes is investigated by density-functional-theory calculations. For the biradicals in benzene, naphthalene, anthracene, tetracene, pentacene, and hexacene, we find that the singlet state is energetically favored over the triplet state by 189, 191, 184, 199, 218, and 244 meV, respectively. The monotonous increase of the singlet-triplet energy gap from anthracene to hexacene is attributed to the enhanced stability of the singlet state for longer polyacenes. Our analysis shows that the spin density of the singlet state is delocalized over all benzene rings, but such a spin delocalization is not present for the triplet state.

Nanosecond time-resolved characterization of a pentacene-based room-temperature MASER

PubMed Central

Salvadori, Enrico; Breeze, Jonathan D.; Tan, Ke-Jie; Sathian, Juna; Richards, Benjamin; Fung, Mei Wai; Wolfowicz, Gary; Oxborrow, Mark; Alford, Neil McN.; Kay, Christopher W. M.

2017-01-01

The performance of a room temperature, zero-field MASER operating at 1.45 GHz has been examined. Nanosecond laser pulses, which are essentially instantaneous on the timescale of the spin dynamics, allow the visible-to-microwave conversion efficiency and temporal response of the MASER to be measured as a function of excitation energy. It is observed that the timing and amplitude of the MASER output pulse are correlated with the laser excitation energy: at higher laser energy, the microwave pulses have larger amplitude and appear after shorter delay than those recorded at lower laser energy. Seeding experiments demonstrate that the output variation may be stabilized by an external source and establish the minimum seeding power required. The dynamics of the MASER emission may be modeled by a pair of first order, non-linear differential equations, derived from the Lotka-Volterra model (Predator-Prey), where by the microwave mode of the resonator is the predator and the spin polarization in the triplet state of pentacene is the prey. Simulations allowed the Einstein coefficient of stimulated emission, the spin-lattice relaxation and the number of triplets contributing to the MASER emission to be estimated. These are essential parameters for the rational improvement of a MASER based on a spin-polarized triplet molecule. PMID:28169331

Low-voltage electron microscopy of polymer and organic molecular thin films.

PubMed

Drummy, Lawrence F; Yang, Junyan; Martin, David C

2004-06-01

We have demonstrated the capabilities of a novel low-voltage electron microscope (LVEM) for imaging polymer and organic molecular thin films. The LVEM can operate in transmission electron microscopy, scanning transmission electron microscopy, scanning electron microscopy, and electron diffraction modes. The microscope operates at a nominal accelerating voltage of 5 kV and fits on a tabletop. A detailed discussion of the electron-sample interaction processes is presented, and the mean free path for total electron scattering was calculated to be 15 nm for organic samples at 5 kV. The total end point dose for the destruction of crystallinity at 5 kV was estimated at 5 x 10(-4) and 3.5 x 10(-2) C/cm2 for polyethylene and pentacene, respectively. These values are significantly lower than those measured at voltages greater than 100 kV. A defocus series of colloidal gold particles allowed us to estimate the experimental contrast transfer function of the microscope. Images taken of several organic materials have shown high contrast for low atomic number elements and a resolution of 2.5 nm. The materials studied here include thin films of the organic semiconductor pentacene, triblock copolymer films, single-molecule dendrimers, electrospun polymer fibers and gold nanoparticles. Copyright 2004 Elsevier B.V.

Elaborately Tuning Intramolecular Electron Transfer Through Varying Oligoacene Linkers in the Bis(diarylamino) Systems

PubMed Central

Zhang, Jing; Chen, Zhao; Yang, Lan; Pan, Fang-Fang; Yu, Guang-Ao; Yin, Jun; Liu, Sheng Hua

2016-01-01

The research efforts on oligoacene systems are still relatively limited mainly due to the synthetic challenge and the extreme instability of longer acenes. Herein, these two issues have been overcome through elaborative modification and the stable pentacene species has been successfully synthesized. Additionally, a series of bis(diarylamino) compounds linked by variable-length oligoacene bridges ranging from one to five fused rings (benzene (1a), naphthalene (1b), anthracene (1c), tetracene (1d) and pentacene (1e)) have been prepared to probe the effect of the extent of π-conjugation on the electron transfer properties. Compound 1c exhibits a high planarity between the anthracyl bridge and the two nitrogen cores and the molecular packing shows a two-dimensional herringbone characteristic. Combined studies based on electrochemistry and spectroelectrochemistry demonstrate that (i) the electronic coupling across the oligoacene linkers between two diarylamine termini exponentially decrease with a moderate attenuation constant (β) of 0.14 Å−1 in these length-modulated systems and (ii) the associated radical cations [1a]+–[1e]+ are classified as the class II Robin–Day mixed-valence systems. Furthermore, density functional theory (DFT) calculations have been conducted to gain insight into the nature of electron transfer processes in these oligoacene systems. PMID:27805023

Experimental investigation on On-Off current ratio behavior near onset voltage for a pentacene based organic thin film transistor

NASA Astrophysics Data System (ADS)

Amrani, Aumeur El; Es-saghiri, Abdeljabbar; Boufounas, El-Mahjoub; Lucas, Bruno

2018-06-01

The performance of a pentacene based organic thin film transistor (OTFT) with polymethylmethacrylate as a dielectric insulator and indium tin oxide based electrical gate is investigated. On the one hand, we showed that the threshold voltage increases with gate voltage, and on the other hand that it decreases with drain voltage. Thus, we noticed that the onset voltage shifts toward positive voltage values with the drain voltage increase. In addition, threshold-onset differential voltage (TODV) is proposed as an original approach to estimate an averaged carrier density in pentacene. Indeed, a value of about 4.5 × 1016 cm-3 is reached at relatively high gate voltage of -50 V; this value is in good agreement with that reported in literature with other technique measurements. However, at a low applied gate voltage, the averaged pentacene carrier density remains two orders of magnitude lower; it is of about 2.8 × 1014 cm-3 and remains similar to that obtained from space charge limited current approach for low applied bias voltage of about 2.2 × 1014 cm-3. Furthermore, high IOn/IOff and IOn/IOnset current ratios of 5 × 106 and 7.5 × 107 are reported for lower drain voltage, respectively. The investigated OTFTs also showed good electrical performance including carrier mobility increasing with gate voltage; mobility values of 4.5 × 10-2 cm2 V-1 s-1 and of 4.25 × 10-2 cm2 V-1 s-1 are reached for linear and saturation regimes, respectively. These results remain enough interesting since current modulation ratio exceeds a value of 107 that is a quite important requirement than high mobility for some particular logic gate applications.

Microscopic studies of the fate of charges in organic semiconductors: Scanning Kelvin probe measurements of charge trapping, transport, and electric fields in p- and n-type devices

NASA Astrophysics Data System (ADS)

Smieska, Louisa Marion

Organic semiconductors could have wide-ranging applications in lightweight, efficient electronic circuits. However, several fundamental questions regarding organic electronic device behavior have not yet been fully addressed, including the nature of chemical charge traps, and robust models for injection and transport. Many studies focus on engineering devices through bulk transport measurements, but it is not always possible to infer the microscopic behavior leading to the observed measurements. In this thesis, we present scanning-probe microscope studies of organic semiconductor devices in an effort to connect local properties with local device behavior. First, we study the chemistry of charge trapping in pentacene transistors. Working devices are doped with known pentacene impurities and the extent of charge trap formation is mapped across the transistor channel. Trap-clearing spectroscopy is employed to measure an excitation of the pentacene charge trap species, enabling identification of the degradationrelated chemical trap in pentacene. Second, we examine transport and trapping in peryelene diimide (PDI) transistors. Local mobilities are extracted from surface potential profiles across a transistor channel, and charge injection kinetics are found to be highly sensitive to electrode cleanliness. Trap-clearing spectra generally resemble PDI absorption spectra, but one derivative yields evidence indicating variation in trap-clearing mechanisms for different surface chemistries. Trap formation rates are measured and found to be independent of surface chemistry, contradicting a proposed silanol trapping mechanism. Finally, we develop a variation of scanning Kelvin probe microscopy that enables measurement of electric fields through a position modulation. This method avoids taking a numeric derivative of potential, which can introduce high-frequency noise into the electric field signal. Preliminary data is presented, and the theoretical basis for electric field noise in both methods is examined.

HED-TIE: A wafer-scale approach for fabricating hybrid electronic devices with trench isolated electrodes

NASA Astrophysics Data System (ADS)

Banerjee, Sreetama; Bülz, Daniel; Solonenko, Dmytro; Reuter, Danny; Deibel, Carsten; Hiller, Karla; Zahn, Dietrich R. T.; Salvan, Georgeta

2017-05-01

Organic-inorganic hybrid electronic devices (HEDs) offer opportunities for functionalities that are not easily obtainable with either organic or inorganic materials individually. In the strive for down-scaling the channel length in planar geometry HEDs, the best results were achieved with electron beam lithography or nanoimprint lithography. Their application on the wafer level is, however, cost intensive and time consuming. Here, we propose trench isolated electrode (TIE) technology as a fast, cost effective, wafer-level approach for the fabrication of planar HEDs with electrode gaps in the range of 100 nm. We demonstrate that the formation of the organic channel can be realized by deposition from solution as well as by the thermal evaporation of organic molecules. To underline one key feature of planar HED-TIEs, namely full accessibility of the active area of the devices by external stimuli such as light, 6,13-bis (triisopropylsilylethynyl) (TIPS)-pentacene/Au HED-TIEs are successfully tested for possible application as hybrid photodetectors in the visible spectral range.

Effect of molecular side groups and local nanoenvironment on photodegradation and its reversibility

NASA Astrophysics Data System (ADS)

Quist, Nicole; Li, Mark; Tollefsen, Ryan; Haley, Michael; Anthony, John; Ostroverkhova, Oksana

2018-02-01

Degradation of organic semiconductors in the presence of oxygen is one of the bottlenecks preventing their wide-spread use in optoelectronic devices. The first step towards such degradation in functionalized pentacene (Pn) derivatives is formation of endoperoxide (EPO), which can either revert back to the parent molecule or proceed to molecule decomposition. We present the study of reversibility of EPO formation through probing the photophysical properties of functionalized fluorinated pentacene (Pn-R-F8) derivatives. Experiments are done in solutions and in films both at the single molecule level and in the bulk. In solutions, degradation of optical absorption and its partial recovery after thermolysis were quantified for various derivatives depending on the solvent. At the single molecule level, low concentrations of each type of molecules were imaged in a variety of polymer matrices at 633 nm excitation at room temperature in air using wide-field fluorescence microscopy. Fluorescence time trajectories were collected and statistically analyzed to quantify blinking due to reversible EPO formation depending on the host matrix. To understand the physical changes of the molecular system, a Monte Carlo method was used to create a multi-level simulation, which enabled us to relate the change in the molecular transition rates to the experimentally measured parameters. At the bulk level, photoluminescence decay due to photobleaching and recovery due to EPO reconversion were measured for the same derivatives incorporated into various matrices. These studies provide insight into the synergistic effect of the local nanoenvironment and molecular side groups on the oxygen-related degradation and subsequent recovery which is important for development of organic electronic devices.

Tensor network methods for the simulation of open quantum dynamics in multichromophore systems: Application to singlet fission in novel pentacene dimers

NASA Astrophysics Data System (ADS)

Chin, Alex

Singlet fission (SF) is an ultrafast process in which a singlet exciton spontaneously converts into a pair of entangled triplet excitons on neighbouring organic molecules. As a mechanism of multiple exciton generation, it has been suggested as a way to increase the efficiency of organic photovoltaic devices, and its underlying photophysics across a wide range of molecules and materials has attracted significant theoretical attention. Recently, a number of studies using ultrafast nonlinear optics have underscored the importance of intramolecular vibrational dynamics in efficient SF systems, prompting a need for methods capable of simulating open quantum dynamics in the presence of highly structured and strongly coupled environments. Here, a combination of ab initio electronic structure techniques and a new tensor-network methodology for simulating open vibronic dynamics is presented and applied to a recently synthesised dimer of pentacene (DP-Mes). We show that ultrafast (300 fs) SF in this system is driven entirely by symmetry breaking vibrations, and our many-body approach enables the real-time identification and tracking of the ''functional' vibrational dynamics and the role of the ''bath''-like parts of the environment. Deeper analysis of the emerging wave functions points to interesting links between the time at which parts of the environment become relevant to the SF process and the optimal topology of the tensor networks, highlighting the additional insight provided by moving the problem into the natural language of correlated quantum states and how this could lead to simulations of much larger multichromophore systems Supported by The Winton Programme for the Physics of Sustainability.

Voltage stress induced reversible diode behavior in pentacene thin films

NASA Astrophysics Data System (ADS)

Murdey, Richard; Sato, Naoki

2012-12-01

The current-voltage characteristics of a vacuum-deposited 100 nm pentacene thin film have been measured in situ under ultrahigh vacuum. Despite using bottom contact geometry with titanium for both electrodes, the I-V curves are asymmetric and the direction and degree of the diode-like behavior vary with sample and measurement history. After careful examination we have found that applying a high positive or negative bias voltage for about 24 h at elevated temperatures was sufficient to completely switch the diode forward direction. The switching action is fully reversible and the diode behavior, once switched, remains stable to repeated measurements at least over a period of several weeks.

Effect of pentacene/Ag anode buffer and UV-ozone treatment on durability of small-molecule organic solar cells

NASA Astrophysics Data System (ADS)

Inagaki, S.; Sueoka, S.; Harafuji, K.

2017-06-01

Three surface modifications of indium tin oxide (ITO) are experimentally investigated to improve the performance of small-molecule organic solar cells (OSCs) with an ITO/anode buffer layer (ABL)/copper phthalocyanine (CuPc)/fullerene/bathocuproine/Ag structure. An ultrathin Ag ABL and ultraviolet (UV)-ozone treatment of ITO independently improve the durability of OSCs against illumination stress. The thin pentacene ABL provides good ohmic contact between the ITO and the CuPc layer, thereby producing a large short-circuit current. The combined use of the abovementioned three modifications collectively achieves both better initial performance and durability against illumination stress.

Highly anisotropic mobility in solution processed TIPS-pentacene film studied by independently driven four GaIn probes

NASA Astrophysics Data System (ADS)

Yoshimoto, Shinya; Takahashi, Kohtaro; Suzuki, Mitsuharu; Yamada, Hiroko; Miyahara, Ryosuke; Mukai, Kozo; Yoshinobu, Jun

2017-08-01

We have studied in-plane anisotropy in the field-effect mobility of solution-processed organic semiconductor 6,13-bis(triisopropylsilylethynyl)pentacene by using independently driven four gallium indium (Ga-In) probes. Liquid-metal Ga-In probes are highly effective for reproducible conductivity measurements of organic thin films. We demonstrated that a high mobility anisotropy of 44 was obtained by using a square four-probe method and a feedback circuit to keep the channel potential constant. The present method minimized the influences of the contact resistance and the insensitivity of anisotropy in a linear arrangement in two-dimensional field-effect transistors.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kowarik, S.; Hinderhofer, A.; Wang, C.

Highly crystalline and stable molecular superlattices are grown with the smallest possible stacking period using monolayers (MLs) of the organic semiconductors pentacene (PEN) and perfluoro-pentacene (PFP). Superlattice reflections in X-ray reflectivity and their energy dependence in resonant soft X-ray reflectivity measurements show that PFP and PEN MLs indeed alternate even though the coherent ordering is lost after ~ 4 ML. The observed lattice spacing of 15.9 Å in the superlattice is larger than in pure PEN and PFP films, presumably because of more upright standing molecules and lack of interdigitation between the incommensurate crystalline PEN and PFP layers. The findingsmore » are important for the development of novel organic quantum optoelectronic devices.« less

Effect of long-range correlation on the metal-insulator transition in a disordered molecular crystal

NASA Astrophysics Data System (ADS)

Unge, Mikael; Stafström, Sven

2006-12-01

Localization lengths of the electronic states in a disordered two-dimensional system, resembling highly anisotropic molecular crystals such as pentacene, have been calculated numerically using the transfer matrix method. The disorder is based on a model with small random fluctuations of induced molecular dipole moments which give rise to long-range correlated disorder in the on-site energies as well as a coupling between the on-site energies and the intermolecular interactions. Our calculations show that molecular crystals such as pentacene can exhibit states with very long localization lengths with a possibility to reach a truly metallic state.

Electrochemical doping for lowering contact barriers in organic field effect transistors

PubMed Central

Schaur, Stefan; Stadler, Philipp; Meana-Esteban, Beatriz; Neugebauer, Helmut; Serdar Sariciftci, N.

2012-01-01

By electrochemically p-doping pentacene in the vicinity of the source-drain electrodes in organic field effect transistors the injection barrier for holes is decreased. The focus of this work is put on the influence of the p-doping process on the transistor performance. Cyclic voltammetry performed on a pentacene based transistor exhibits a reversible p-doping response. This doped state is evoked at the transistor injection electrodes. An improvement is observed when comparing transistor characteristics before and after the doping process apparent by an improved transistor on-current. This effect is reflected in the analysis of the contact resistances of the devices. PMID:23483101

Grain Boundary Effect on Charge Transport in Pentacene Thin Films

NASA Astrophysics Data System (ADS)

Weis, Martin; Gmucová, Katarína; Nádaždy, Vojtech; Majková, Eva; Haško, Daniel; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2011-04-01

We report on charge transport properties of polycrystalline pentacene films with variable average grain size in the range from 0.1 to 0.3 µm controlled by the preparation technology. We illustrate with the organic field-effect transistors decrease of the effective mobility and presence of traps with decrease of the grain size. Analysis of the charge transfer excitons reveals decrease of the mobile charge density and the steady-state voltammetry showed significant increase of oxygen- and hydrogen-related defects. We also briefly discuss accumulation of the defects on the grain boundary and show relation between the defect density and grain boundary length.

Thermionic emission and tunneling at carbon nanotube-organic semiconductor interface.

PubMed

Sarker, Biddut K; Khondaker, Saiful I

2012-06-26

We study the charge carrier injection mechanism across the carbon nanotube (CNT)-organic semiconductor interface using a densely aligned carbon nanotube array as electrode and pentacene as organic semiconductor. The current density-voltage (J-V) characteristics measured at different temperatures show a transition from a thermal emission mechanism at high temperature (above 200 K) to a tunneling mechanism at low temperature (below 200 K). A barrier height of ∼0.16 eV is calculated from the thermal emission regime, which is much lower compared to the metal/pentacene devices. At low temperatures, the J-V curves exhibit a direct tunneling mechanism at low bias, corresponding to a trapezoidal barrier, while at high bias the mechanism is well described by Fowler-Nordheim tunneling, which corresponds to a triangular barrier. A transition from direct tunneling to Fowler-Nordheim tunneling further signifies a small injection barrier at the CNT/pentacene interface. Our results presented here are the first direct experimental evidence of low charge carrier injection barrier between CNT electrodes and an organic semiconductor and are a significant step forward in realizing the overall goal of using CNT electrodes in organic electronics.

Composite fluorescent nanoparticles for biomedical imaging.

PubMed

Pansare, Vikram J; Bruzek, Matthew J; Adamson, Douglas H; Anthony, John; Prud'homme, Robert K

2014-04-01

In the rapidly expanding field of biomedical imaging, there is a need for nontoxic, photostable, and nonquenching fluorophores for fluorescent imaging. We have successfully encapsulated a new, extremely hydrophobic, pentacene-based fluorescent dye within polymeric nanoparticles (NPs) or nanocarriers (NCs) via the Flash NanoPrecipitation (FNP) process. Nanoparticles and dye-loaded micelles were formulated by FNP and characterized by dynamic light scattering, fluorescence spectroscopy, UV-VIS absorbance spectroscopy, and confocal microscopy. These fluorescent particles were loaded from less than 1% to 78% by weight core loading and the fluorescence maximum was found to be at 2.3 wt.%. The particles were also stably formed at 2.3% core loading from 20 up to 250 nm in diameter with per-particle fluorescence scaling linearly with the NC core volume. The major absorption peaks are at 458, 575, and 625 nm, and the major emission peaks at 635 and 695 nm. In solution, the Et-TP5 dye displays a strong concentration-dependent ratio of the emission intensities of the first two emission peaks, whereas in the nanoparticle core the spectrum is independent of concentration over the entire concentration range. A model of the fluorescence quenching was consistent with Förster resonant energy transfer as the cause of the quenching observed for Et-TP5. The Förster radius calculated from the absorption and emission spectra of Et-TP5 is 4.1 nm, whereas the average dye spacing in the particles at the maximum fluorescence is 3.9 nm. We have successfully encapsulated Et-TP5, a pentacene derivative dye previously only used in light-emitting diode applications, within NCs via the FNP process. The extreme hydrophobicity of the dye keeps it encapsulated in the NC core, its extended pentacene structure gives it relatively long wavelength emission at 695 nm, and the pentacene structure, without oxygen or nitrogen atoms in its core, makes it highly resistant to photobleaching. Its bulky side groups minimize self-quenching and localization within the nanoparticle core prevents interaction of the dye with biological surfaces, or molecules in diagnostic assays. Loading of dye in the NP core allows 25 times more dye to be delivered than if it were conjugated onto the nanocarrier surface. The utility of the dye for quantifying nanoparticle binding is demonstrated. Studies to extend the wavelength range of these pentacene dyes into the near infra-red are underway.

Theoretical studies of growth processes and electronic properties of nanostructures on surfaces

NASA Astrophysics Data System (ADS)

Mo, Yina

Low dimensional nanostructures have been of particular interest because of their potential applications in both theoretical studies and industrial use. Although great efforts have been put into obtaining better understanding of the formation and properties of these materials, many questions still remain unanswered. This thesis work has focused on theoretical studies of (1) the growth processes of magnetic nanowires on transition-metal surfaces, (2) the dynamics of pentacene thin-film growth and island structures on inert surfaces, and (3) our proposal of a new type of semiconducting nanotube. In the first study, we elucidated a novel and intriguing kinetic pathway for the formation of Fe nanowires on the upper edge of a monatomic-layer-high step on Cu(111) using first-principles calculations. The identification of a hidden fundamental Fe basal line within the Cu steps prior to the formation of the apparent upper step edge Fe wire produces a totally different view of step-decorating wire structures and offers new possibilities for the study of the properties of these wires. Subsequent experiments with scanning tunneling microscopy unambiguously established the essential role of embedded Fe atoms as precursors to monatomic wire growth. A more general study of adatom behavior near transition-metal step edges illustrated a systematic trend in the adatom energetics and kinetics, resulted from the electronic interactions between the adatom and the surfaces. This work opens the possibility of controlled manufacturing of one-dimensional nanowires. In the second study, we investigated pentacene thin-films on H-diamond, H-silica and OH-silica surfaces via force field molecular dynamics simulations. Pentacene island structures on these surfaces were identified and found to have a 90-degree rotation relative to the structure proposed by some experimental groups. Our work may facilitate the design and control of experimental pentacene thin-film growth, and thus the development of organic thin-film transistors. Finally, in our third study, we proposed a new type of structurally simple and energetically stable cyanide transition metal nanotube, based on the planar structure of M(CN)2, (M = Ni, Pd, Pt). These nanotubes have semiconducting character with large band gaps (2--3 eV), which are insensitive to the chirality and diameter. We have investigated the energetic, electronic, and mechanical properties of these materials in both planar and tubular forms through first-principles density functional calculations. These calculations reveal interesting multi-center bonding features that should lead to preferential growth of tubes of a particular chirality. The unique features of these nanotubes should make them capable of being mass-produced, which is one of the most significant shortcomings of semiconducting carbon nanotubes.

Up-regulation of CYP1A1 and phase II enzymes by 5-ring isomeric polycyclic aromatic hydrocarbons in precision-cut rat hepatic slices: Importance of molecular shape.

PubMed

Pushparajah, Daphnee; Lewis, Dfv; Ioannides, Costas

2017-04-01

The objectives of the present study were two-fold: (a) to evaluate the role of molecular shape on the interaction of polycyclic aromatic hydrocarbons (PAHs) with the Ah receptor and CYP1A1 upregulation, and (b) to evaluate the potential of PAHs to induce epoxide hydrolase and glutathione S-transferase, two major enzymes involved in their metabolism. In order to achieve these objectives, precision-cut rat liver slices were incubated with a range of concentrations of seven 5-ring isomeric PAHs, namely benzo[c]chrysene, benzo[b]chrysene, benzo[g]chrysene, dibenzo[a,j]anthracene, dibenzo[a,c]anthracene, picene and pentacene, for 24h. All compounds, with the exception of pentacene, elevated the O-deethylation of ethoxyresorufin, an activity associated with CYP1A1; induction of this enzyme by the various PAHs correlated with their avidity for the Ah receptor. None of the PAHs studied increased epoxide hydrolase activity, monitored using benzo[a]pyrene 4,5-oxide. Of the seven PAHs, only benzo[g]chrysene elevated glutathione S-transferase activity, measured using 1-chloro-2,4-dinitrobenzene or 7-chloro-4-nitrobenzo-2-oxa-1,3-diazole as substrates. No relationship could be established between length or length/width and interaction with the Ah receptor and CYP1A1 up-regulation indicating that other structural or electronic factors are likely to be more important. Finally, 5-ring PAHs are poor inducers of the epoxide hydrolase and glutathione S-transferase enzyme systems. Copyright © 2017 Elsevier Ltd. All rights reserved.

A nanoscale study of charge extraction in organic solar cells: the impact of interfacial molecular configurations.

PubMed

Tang, Fu-Ching; Wu, Fu-Chiao; Yen, Chia-Te; Chang, Jay; Chou, Wei-Yang; Gilbert Chang, Shih-Hui; Cheng, Horng-Long

2015-01-07

In the optimization of organic solar cells (OSCs), a key problem lies in the maximization of charge carriers from the active layer to the electrodes. Hence, this study focused on the interfacial molecular configurations in efficient OSC charge extraction by theoretical investigations and experiments, including small molecule-based bilayer-heterojunction (sm-BLHJ) and polymer-based bulk-heterojunction (p-BHJ) OSCs. We first examined a well-defined sm-BLHJ model system of OSC composed of p-type pentacene, an n-type perylene derivative, and a nanogroove-structured poly(3,4-ethylenedioxythiophene) (NS-PEDOT) hole extraction layer. The OSC with NS-PEDOT shows a 230% increment in the short circuit current density compared with that of the conventional planar PEDOT layer. Our theoretical calculations indicated that small variations in the microscopic intermolecular interaction among these interfacial configurations could induce significant differences in charge extraction efficiency. Experimentally, different interfacial configurations were generated between the photo-active layer and the nanostructured charge extraction layer with periodic nanogroove structures. In addition to pentacene, poly(3-hexylthiophene), the most commonly used electron-donor material system in p-BHJ OSCs was also explored in terms of its possible use as a photo-active layer. Local conductive atomic force microscopy was used to measure the nanoscale charge extraction efficiency at different locations within the nanogroove, thus highlighting the importance of interfacial molecular configurations in efficient charge extraction. This study enriches understanding regarding the optimization of the photovoltaic properties of several types of OSCs by conducting appropriate interfacial engineering based on organic/polymer molecular orientations. The ultimate power conversion efficiency beyond at least 15% is highly expected when the best state-of-the-art p-BHJ OSCs are combined with present arguments.

Silicone substrate with in situ strain relief for stretchable thin-film transistors

NASA Astrophysics Data System (ADS)

Graz, Ingrid M.; Cotton, Darryl P. J.; Robinson, Adam; Lacour, Stéphanie P.

2011-03-01

We have manufactured stretchable thin-film transistors and interconnects directly onto an engineered silicone matrix with localized and graded mechanical compliance. The fabrication only involves planar and standard processing. Brittle active device materials are patterned on non deformable elastomer regions (strain <1% at all times) while interconnects run smoothly from "stiff" to "soft" elastomer. Pentacene thin-film transistors sustain applied strain up to 13% without electrical degradation and mechanical fracture. This integrated approach opens promising options for the manufacture of physically adaptable and transformable circuitry.

Solution processed molecular floating gate for flexible flash memories

NASA Astrophysics Data System (ADS)

Zhou, Ye; Han, Su-Ting; Yan, Yan; Huang, Long-Biao; Zhou, Li; Huang, Jing; Roy, V. A. L.

2013-10-01

Solution processed fullerene (C60) molecular floating gate layer has been employed in low voltage nonvolatile memory device on flexible substrates. We systematically studied the charge trapping mechanism of the fullerene floating gate for both p-type pentacene and n-type copper hexadecafluorophthalocyanine (F16CuPc) semiconductor in a transistor based flash memory architecture. The devices based on pentacene as semiconductor exhibited both hole and electron trapping ability, whereas devices with F16CuPc trapped electrons alone due to abundant electron density. All the devices exhibited large memory window, long charge retention time, good endurance property and excellent flexibility. The obtained results have great potential for application in large area flexible electronic devices.

An efficient strategy for designing ambipolar organic semiconductor material: Introducing dehydrogenated phosphorus atoms into pentacene core

NASA Astrophysics Data System (ADS)

Tang, Xiao-Dan

2017-09-01

The charge transport properties of phosphapentacene (P-PEN) derivatives were systematically explored by theoretical calculation. The dehydrogenated P-PENs have reasonable frontier molecular orbital energy levels to facilitate both electron and hole injection. The reduced reorganization energies of dehydrogenated P-PENs could be intimately connected to the bonding nature of phosphorus atoms. From the idea of homology modeling, the crystal structure of TIPSE-4P-2p is constructed and fully optimized. Fascinatingly, TIPSE-4P-2p shows the intrinsic property of ambipolar transport in both hopping and band models. Thus, introducing dehydrogenated phosphorus atoms into pentacene core could be an efficient strategy for designing ambipolar material.

Pentacene-based metal-insulator-semiconductor memory structures utilizing single walled carbon nanotubes as a nanofloating gate

NASA Astrophysics Data System (ADS)

Sleiman, A.; Rosamond, M. C.; Alba Martin, M.; Ayesh, A.; Al Ghaferi, A.; Gallant, A. J.; Mabrook, M. F.; Zeze, D. A.

2012-01-01

A pentacene-based organic metal-insulator-semiconductor memory device, utilizing single walled carbon nanotubes (SWCNTs) for charge storage is reported. SWCNTs were embedded, between SU8 and polymethylmethacrylate to achieve an efficient encapsulation. The devices exhibit capacitance-voltage clockwise hysteresis with a 6 V memory window at ± 30 V sweep voltage, attributed to charging and discharging of SWCNTs. As the applied gate voltage exceeds the SU8 breakdown voltage, charge leakage is induced in SU8 to allow more charges to be stored in the SWCNT nodes. The devices exhibited high storage density (˜9.15 × 1011 cm-2) and demonstrated 94% charge retention due to the superior encapsulation.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Roth, Friedrich, E-mail: Friedrich.Roth@cfel.de; Knupfer, Martin, E-mail: M.Knupfer@ifw-dresden.de

We report the doping induced changes of the electronic structure of tetracene and pentacene probed by electron energy-loss spectroscopy in transmission. A comparison between the dynamic response of undoped and potassium-intercalated tetracene and pentacene emphasizes the appearance of a new excitation feature in the former gap upon potassium addition. Interestingly, the momentum dependency of this new excitation shows a negative dispersion. Moreover, the analysis of the C 1s and K 2p core-level excitation results in a significantly lower doping level compared to potassium doped picene, a recently discovered superconductor. Therefore, the present electronic structure investigations open a new pathway to better understandmore » the exceptional differences between acenes and phenacene and their divergent behavior upon alkali doping.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kowarik, S.; Weber, C.; Hinderhofer, A.

Highly crystalline and stable molecular superlattices are grown with the smallest possible stacking period using monolayers (MLs) of the organic semiconductors pentacene (PEN) and perfluoro-pentacene (PFP). Superlattice reflections in X-ray reflectivity and their energy dependence in resonant soft X-ray reflectivity measurements show that PFP and PEN MLs indeed alternate even though the coherent ordering is lost after ∼ 4 ML. The observed lattice spacing of 15.9 Å in the superlattice is larger than in pure PEN and PFP films, presumably because of more upright standing molecules and lack of interdigitation between the incommensurate crystalline PEN and PFP layers. The findingsmore » are important for the development of novel organic quantum optoelectronic devices.« less

Solution processed molecular floating gate for flexible flash memories

PubMed Central

Zhou, Ye; Han, Su-Ting; Yan, Yan; Huang, Long-Biao; Zhou, Li; Huang, Jing; Roy, V. A. L.

2013-01-01

Solution processed fullerene (C60) molecular floating gate layer has been employed in low voltage nonvolatile memory device on flexible substrates. We systematically studied the charge trapping mechanism of the fullerene floating gate for both p-type pentacene and n-type copper hexadecafluorophthalocyanine (F16CuPc) semiconductor in a transistor based flash memory architecture. The devices based on pentacene as semiconductor exhibited both hole and electron trapping ability, whereas devices with F16CuPc trapped electrons alone due to abundant electron density. All the devices exhibited large memory window, long charge retention time, good endurance property and excellent flexibility. The obtained results have great potential for application in large area flexible electronic devices. PMID:24172758

Calculating the trap density of states in organic field-effect transistors from experiment: A comparison of different methods

NASA Astrophysics Data System (ADS)

Kalb, Wolfgang L.; Batlogg, Bertram

2010-01-01

The spectral density of localized states in the band gap of pentacene (trap DOS) was determined with a pentacene-based thin-film transistor from measurements of the temperature dependence and gate-voltage dependence of the contact-corrected field-effect conductivity. Several analytical methods to calculate the trap DOS from the measured data were used to clarify, if the different methods lead to comparable results. We also used computer simulations to further test the results from the analytical methods. Most methods predict a trap DOS close to the valence-band edge that can be very well approximated by a single exponential function with a slope in the range of 50-60 meV and a trap density at the valence-band edge of ≈2×1021eV-1cm-3 . Interestingly, the trap DOS is always slightly steeper than exponential. An important finding is that the choice of the method to calculate the trap DOS from the measured data can have a considerable effect on the final result. We identify two specific simplifying assumptions that lead to significant errors in the trap DOS. The temperature dependence of the band mobility should generally not be neglected. Moreover, the assumption of a constant effective accumulation-layer thickness leads to a significant underestimation of the slope of the trap DOS.

Effects of different self-assembled monolayers on thin-film morphology: a combined DFT/MD simulation protocol.

PubMed

Alberga, Domenico; Mangiatordi, Giuseppe Felice; Motta, Alessandro; Nicolotti, Orazio; Lattanzi, Gianluca

2015-10-06

Organic thin film transistors (OTFTs) are multilayer field-effect transistors that employ an organic conjugated material as semiconductor. Several experimental groups have recently demonstrated that the insertion of an organic self-assembled monolayer (SAM) between the dielectric and the semiconductive layer is responsible for a sensible improvement of the OTFT performances in terms of an increased charge carrier mobility caused by a higher degree of order in the organic semiconductor layer. Here, we describe a combined periodic density functional theory (DFT) and classical molecular dynamics (MD) protocol applied to four different SAMs and a pentacene monolayer deposited onto their surfaces. In particular, we investigate the morphology and the surface of the four SAMs and the translational, orientational, and nematic order of the monolayer through the calculation of several distribution functions and order parameters pointing out the differences among the systems and relating them to known experimental results. Our calculations also suggest that small differences in the SAM molecular design will produce remarkable differences in the SAM surface and monolayer order. In particular, our simulations explain how a SAM with a bulky terminal group results in an irregular and rough surface that determines the deposition of a disordered semiconductive monolayer. On the contrary, SAMs with a small terminal group generate smooth surfaces with uninterrupted periodicity, thus favoring the formation of an ordered pentacene monolayer that increases the mobility of charge carriers and improves the overall performances of the OTFT devices. Our results clearly point out that the in silico procedure presented here might be of help in tuning the design of SAMs in order to improve the quality of OTFT devices.

Site energies and charge transfer rates near pentacene grain boundaries from first-principles calculations

NASA Astrophysics Data System (ADS)

Kobayashi, Hajime; Tokita, Yuichi

2015-03-01

Charge transfer rates near pentacene grain boundaries are derived by calculating the site energies and transfer integrals of 37 pentacene molecules using first-principles calculations. The site energies decrease considerably near the grain boundaries, and electron traps of up to 300 meV and hole barriers of up to 400 meV are generated. The charge transfer rates across the grain boundaries are found to be reduced by three to five orders of magnitude with a grain boundary gap of 4 Å because of the reduction in the transfer integrals. The electron traps and hole barriers also reduce the electron and hole transfer rates by factors of up to 10 and 50, respectively. It is essential to take the site energies into consideration to determine charge transport near the grain boundaries. We show that the complex site energy distributions near the grain boundaries can be represented by an equivalent site energy difference, which is a constant for any charge transfer pass. When equivalent site energy differences are obtained for various grain boundary structures by first-principles calculations, the effects of the grain boundaries on the charge transfer rates are introduced exactly into charge transport simulations, such as the kinetic Monte Carlo method.

Achieving high mobility, low-voltage operating organic field-effect transistor nonvolatile memory by an ultraviolet-ozone treating ferroelectric terpolymer

PubMed Central

Xiang, Lanyi; Wang, Wei; Xie, Wenfa

2016-01-01

Poly(vinylidene fluoride–trifluoroethylene) has been widely used as a dielectric of the ferroelectric organic field-effect transistor (FE-OFET) nonvolatile memory (NVM). Some critical issues, including low mobility and high operation voltage, existed in these FE-OFET NVMs, should be resolved before considering to their commercial application. In this paper, we demonstrated low-voltage operating FE-OFET NVMs based on a ferroelectric terpolymer poly(vinylidene-fluoride-trifluoroethylene-chlorotrifluoroethylene) [P(VDF-TrFE-CTFE)] owed to its low coercive field. By applying an ultraviolet-ozone (UVO) treatment to modify the surface of P(VDF-TrFE-CTFE) films, the growth model of the pentacene film was changed, which improved the pentacene grain size and the interface morphology of the pentacene/P(VDF-TrFE-CTFE). Thus, the mobility of the FE-OFET was significantly improved. As a result, a high performance FE-OFET NVM, with a high mobility of 0.8 cm2 V−1 s−1, large memory window of 15.4~19.2, good memory on/off ratio of 103, the reliable memory endurance over 100 cycles and stable memory retention ability, was achieved at a low operation voltage of ±15 V. PMID:27824101

Nonlocal electron-phonon coupling in the pentacene crystal: Beyond the Γ-point approximation

NASA Astrophysics Data System (ADS)

Yi, Yuanping; Coropceanu, Veaceslav; Brédas, Jean-Luc

2012-10-01

There is currently increasing interest in understanding the impact of the nonlocal (Peierls-type) electron-phonon mechanism on charge transport in organic molecular semiconductors. Most estimates of the non-local coupling constants reported in the literature are based on the Γ-point phonon modes. Here, the influence of phonon modes spanning the entire Brillouin zone (phonon dispersion) on the nonlocal electron-phonon couplings is investigated for the pentacene crystal. The phonon modes are obtained by using a supercell approach. The results underline that the overall nonlocal couplings are substantially underestimated by calculations taking sole account of the phonons at the Γ point of the unit cell. The variance of the transfer integrals based on Γ-point normal-mode calculations at room temperature is underestimated in some cases by 40% for herringbone-type dimers and by over 80% for cofacial dimers. Our calculations show that the overall coupling is somewhat larger for holes than for electrons. The results also suggest that the interactions of charge carriers (both electrons and holes) with acoustic and optical phonons are comparable. Therefore, an adequate description of the charge-transport properties in pentacene and similar systems requires that these two electron-phonon coupling mechanisms be treated on the same footing.

A Silicon–Singlet Fission Tandem Solar Cell Exceeding 100% External Quantum Efficiency with High Spectral Stability

PubMed Central

2017-01-01

After 60 years of research, silicon solar cell efficiency saturated close to the theoretical limit, and radically new approaches are needed to further improve the efficiency. The use of tandem systems raises this theoretical power conversion efficiency limit from 34% to 45%. We present the advantageous spectral stability of using voltage-matched tandem solar cells with respect to their traditional series-connected counterparts and experimentally demonstrate how singlet fission can be used to produce simple voltage-matched tandems. Our singlet fission silicon–pentacene tandem solar cell shows efficient photocurrent addition. This allows the tandem system to benefit from carrier multiplication and to produce an external quantum efficiency exceeding 100% at the main absorption peak of pentacene. PMID:28261671

Control of droplet morphology for inkjet-printed TIPS-pentacene transistors

USGS Publications Warehouse

Lee, Myung Won; Ryu, Gi Seong; Lee, Young Uk; Pearson, Christopher; Petty, Michael C.; Song, Chung Kun

2012-01-01

We report on methods to control the morphology of droplets of 6,13-bis(triisopropyl-silylethynyl) pentacene (TIPS-PEN), which are then used in the fabrication of organic thin film transistors (OTFTs). The grain size and distribution of the TIPS-PEN were found to depend on the temperature of the droplets during drying. The performance of the OTFTs could be improved by heating the substrate and also by changing the relative positions of the inkjet-printed droplets. In our experiments, the optimum substrate temperature was 46 °C in air. Transistors with the TIPS-PEN grain boundaries parallel to the current flow between the source and drain electrodes exhibited charge carrier mobilities of 0.44 ± 0.08 cm2/V s.

Top-Contact Pentacene-Based Organic Thin Film Transistor (OTFT) with N, N'-Bis(3-Methyl Phenyl)- N, N'-Diphenyl Benzidine (TPD)/Au Bilayer Source-Drain Electrode

NASA Astrophysics Data System (ADS)

Borthakur, Tribeni; Sarma, Ranjit

2018-01-01

A top-contact Pentacene-based organic thin film transistor (OTFT) with N, N'-Bis (3-methyl phenyl)- N, N'-diphenyl benzidine (TPD)/Au bilayer source-drain electrode is reported. The devices with TPD/Au bilayer source-drain (S-D) electrodes show better performance than the single layer S-D electrode OTFT devices. The field-effect mobility of 4.13 cm2 v-1 s-1, the on-off ratio of 1.86 × 107, the threshold voltage of -4 v and the subthreshold slope of .27 v/decade, respectively, are obtained from the device with a TPD/Au bilayer source-drain electrode.

Hybrid Organic/ZnO p-n Junctions with n-Type ZnO Grown by Atomic Layer Deposition

NASA Astrophysics Data System (ADS)

Łuka, G.; Krajewski, T.; Szczerbakow, A.; Łusakowska, E.; Kopalko, K.; Guziewicz, E.; Wachnicki, Ł.; Szczepanik, A.; Godlewski, M.; Fidelus, J. D.

2008-11-01

We report on fabrication of hybrid inorganic-on-organic thin film structures with polycrystalline zinc oxide films grown by atomic layer deposition technique. ZnO films were deposited on two kinds of thin organic films, i.e. pentacene and poly(dimethylosiloxane) elastomer with a carbon nanotube content (PDMS:CNT). Surface morphology as well as electrical measurements of the films and devices were analyzed. The current density versus voltage (I-V) characteristics of ITO/pentacene/ZnO/Au structure show a low-voltage switching phenomenon typical of organic memory elements. The I-V studies of ITO/PDMS:CNT/ZnO/Au structure indicate some charging effects in the system under applied voltages.

Application of double-hybrid density functionals to charge transfer in N-substituted pentacenequinones.

PubMed

Sancho-García, J C

2012-05-07

A set of N-heteroquinones, deriving from oligoacenes, have been recently proposed as n-type organic semiconductors with high electron mobilities in thin-film transistors. Generally speaking, this class of compounds self-assembles in neighboring π-stacks linked by weak hydrogen bonds. We aim at theoretically characterizing here the sequential charge transport (hopping) process expected to take place across these arrays of molecules. To do so, we need to accurately address the preferred packing of these materials simultaneously to single-molecule properties related to charge-transfer events, carefully employing dispersion-corrected density functional theory methods to accurately extract the key molecular parameters governing this phenomenon at the nanoscale. This study confirms the great deal of interest around these compounds, since controlled functionalization of model molecules (i.e., pentacene) allows to efficiently tune the corresponding charge mobilities, and the capacity of modern quantum-chemical methods to predict it after rationalizing the underlying structure-property relationships.

Organic memory device with self-assembly monolayered aptamer conjugated nanoparticles

NASA Astrophysics Data System (ADS)

Oh, Sewook; Kim, Minkeun; Kim, Yejin; Jung, Hunsang; Yoon, Tae-Sik; Choi, Young-Jin; Jung Kang, Chi; Moon, Myeong-Ju; Jeong, Yong-Yeon; Park, In-Kyu; Ho Lee, Hyun

2013-08-01

An organic memory structure using monolayered aptamer conjugated gold nanoparticles (Au NPs) as charge storage nodes was demonstrated. Metal-pentacene-insulator-semiconductor device was adopted for the non-volatile memory effect through self assembly monolayer of A10-aptamer conjugated Au NPs, which was formed on functionalized insulator surface with prostate-specific membrane antigen protein. The capacitance versus voltage (C-V) curves obtained for the monolayered Au NPs capacitor exhibited substantial flat-band voltage shift (ΔVFB) or memory window of 3.76 V under (+/-)7 V voltage sweep. The memory device format can be potentially expanded to a highly specific capacitive sensor for the aptamer-specific biomolecule detection.

A simple process based on NH2- and CH3-terminated monolayers for low contact resistance and adherent Au electrode in bottom-contact OTFTs

NASA Astrophysics Data System (ADS)

Abdur, Rahim; Lim, Jeongeun; Jeong, Kyunghoon; Rahman, Mohammad Arifur; Kim, Jiyoung; Lee, Jaegab

2016-03-01

An efficient process for the low contact resistance and adherent source/drain Au electrode in bottom-contact organic thin film transistors (OTFTs) was developed. This was achieved by using two different surface-functional groups of self-assembled monolayers, 3-aminopropyltriethoxysilane (APS), and octadecyltrichlorosilane (OTS), combined with atmospheric-pressure (AP) plasma treatment. Prior to the deposition of Au electrode, the aminoterminated monolayer self-assembles on SiO2 dielectrics, enhancing the adhesion of Au electrode as a result of the acid-base interaction of Au with the amino-terminal groups. AP plasma treatment of the patterned Au electrode on the APS-coated surface activates the entire surface to form an OTS monolayer, allowing the formation of a high quality pentacene layer on both the electrode and active region by evaporation. In addition, negligible damage by AP plasma was observed for the device performance. The fabricated OTFTs based on the two monolayers by AP plasma treatment showed the mobility of 0.23 cm2/Vs, contact resistance of 29 kΩ-cm, threshold voltage of -1.63 V, and on/off ratio of 9.8 × 105, demonstrating the application of the simple process for robust and high-performance OTFTs. [Figure not available: see fulltext.

Molecular Imaging of Ultrathin Pentacene Films: Evidence for Homoepitaxy

NASA Astrophysics Data System (ADS)

Wu, Yanfei; Haugstad, Greg; Frisbie, C. Daniel

2013-03-01

Ultrathin polycrystalline films of organic semiconductors have received intensive investigations due to the critical role they play in governing the performance of organic thin film transistors. In this work, a variety of scanning probe microscopy (SPM) techniques have been employed to investigate ultrathin polycrystalline films (1-3 nm) of the benchmark organic semiconductor pentacene. By using spatially resolved Friction Force Microscopy (FFM), Kelvin Probe Force Microscopy (KFM) and Electrostatic Force Microscopy (EFM), an interesting multi-domain structure is revealed within the second layer of the films, characterized as two distinct friction and surface potential domains correlating with each other. The existence of multiple homoepitaxial modes within the films is thus proposed and examined. By employing lattice-revolved imaging using contact mode SPM, direct molecular evidence for the unusual homoepitaxy is obtained.

Nonlinear ultrafast optical response in organic molecular crystals

NASA Astrophysics Data System (ADS)

Rahman, Talat S.; Turkowski, Volodymyr; Leuenberger, Michael N.

2012-02-01

We analyze possible nonlinear excitonic effects in the organic molecule crystals by using a combined time-dependent DFT and many-body approach. In particular, we analyze possible effects of the time-dependent (retarded)interaction between different types of excitations, Frenkel excitons, charge transfer excitons and excimers, on the electric and the optical response of the system. We pay special attention to the case of constant electric field and ultrafast pulses, including that of four-wave mixing experiments. As a specific application we examine the optical excitations of pentacene nanocrystals and compare the results with available experimental data.[1] Our results demostrate that the nonlinear effects can play an important role in the optical response of these systems. [1] A. Kabakchiev, ``Scanning Tunneling Luminescence of Pentacene Nanocrystals'', PhD Thesis (EPFL, Lausanne, 2010).

Morphological and crystalline characterization of pulsed laser deposited pentacene thin films for organic transistor applications

NASA Astrophysics Data System (ADS)

Pereira, Antonio; Bonhommeau, Sébastien; Sirotkin, Sergey; Desplanche, Sarah; Kaba, Mamadouba; Constantinescu, Catalin; Diallo, Abdou Karim; Talaga, David; Penuelas, Jose; Videlot-Ackermann, Christine; Alloncle, Anne-Patricia; Delaporte, Philippe; Rodriguez, Vincent

2017-10-01

We show that high-quality pentacene (P5) thin films of high crystallinity and low surface roughness can be produced by pulsed laser deposition (PLD) without inducing chemical degradation of the molecules. By using Raman spectroscopy and X-ray diffraction measurements, we also demonstrate that the deposition of P5 on Au layers result in highly disordered P5 thin films. While the P5 molecules arrange within the well-documented 1.54-nm thin-film phase on high-purity fused silica substrates, this ordering is indeed destroyed upon introducing an Au interlayer. This observation may be one explanation for the low electrical performances measured in P5-based organic thin film transistors (OTFTs) deposited by laser-induced forward transfer (LIFT).

Post annealing effects on the electrical characteristics of pentacene thin film transistors on flexible substrates.

PubMed

Oh, Tae-Yeon; Jeong, Shin Woo; Chang, Seongpil; Park, Jung-Ho; Kim, Jong-Woo; Choi, Kookhyun; Ha, Hyeon-Jun; Hwang, Bo-Yeon; Ju, Byeong-Kwon

2013-05-01

This work studies the effect of post annealing of pentacene on a flexible substrate through the examination of electrical properties and surface morphologies. It is confirmed that the best performance of devices is achieved when the post annealing temperature is 60 degrees C, since the grain size increases, which decrease grain boundaries caused charge transport limit. We can also confirmed the large threshold voltage shift of device annealed at 60 degrees C that means the lower trap density between channel and insulator interface. The device annealed at 60 degrees C exhibits a saturation mobility of 1.99 cm2/V x s, an on/off ratio of 1.87 x 10(4), and a subthreshold slope of 2.5 V/decade.

Impact of Illumination on Charge Injection and Accumulation in Organic Transistor in Presence of Plasmonic Nanoparticles

NASA Astrophysics Data System (ADS)

Lee, Keanchuan; Weis, Martin; Chen, Xiangyu; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2013-04-01

Effects of illumination on the carrier injection and transport due to photogenerated carriers were investigated in pentacene organic field-effect transistor (OFET). A plasmonic nanoparticles self-assembled monolayer (SAM) was incorporated in pentacene FET to act to enhance the photo-carrier generation. The influence of nanoparticles (NPs) on the photogeneration as well as on the charge trapping has been investigated using the current-voltage (I-V) and impedance spectroscopy (IS) measurements. The I-V results proved higher amount of photogenerated charge in presence of NPs even though this device has the contact resistance about two orders higher and effective mobility an order lower than the reference device without plasmonic NPs. The IS analysis of relaxation times verified strong influence of NPs on the charge trapping.

High-mobility and low-operating voltage organic thin film transistor with epoxy based siloxane binder as the gate dielectric

NASA Astrophysics Data System (ADS)

Tewari, Amit; Gandla, Srinivas; Pininti, Anil Reddy; Karuppasamy, K.; Böhm, Siva; Bhattacharyya, Arup R.; McNeill, Christopher R.; Gupta, Dipti

2015-09-01

This paper reports the fabrication of pentacene-based organic thin-film transistors using a dielectric material, Dynasylan ®SIVO110. The devices exhibit excellent performance characterized by a low threshold voltage of -1.4 V (operating voltage: 0 to -4 V) together with a mobility of 1.9 cm2 V-1s-1. These results are promising because it uses only a single layer of dielectric without performing any intermediate treatment. The reason is attributed to the high charge storage capacity of the dielectric (κ ˜ 20.02), a low interfacial trap density (2.56 × 1011cm-2), and favorable pentacene film morphology consisting of large and interconnected grains having an average size of 234 nm.

NMR shifts for polycyclic aromatic hydrocarbons from first-principles

NASA Astrophysics Data System (ADS)

Thonhauser, T.; Ceresoli, Davide; Marzari, Nicola

We present first-principles, density-functional theory calculations of the NMR chemical shifts for polycyclic aromatic hydrocarbons, starting with benzene and increasing sizes up to the one- and two-dimensional infinite limits of graphene ribbons and sheets. Our calculations are performed using a combination of the recently developed theory of orbital magnetization in solids, and a novel approach to NMR calculations where chemical shifts are obtained from the derivative of the orbital magnetization with respect to a microscopic, localized magnetic dipole. Using these methods we study on equal footing the 1H and 13 shifts in benzene, pyrene, coronene, in naphthalene, anthracene, naphthacene, and pentacene, and finally in graphene, graphite, and an infinite graphene ribbon. Our results show very good agreement with experiments and allow us to characterize the trends for the chemical shifts as a function of system size.

Lateral and Vertical Organic Transistors

NASA Astrophysics Data System (ADS)

Al-Shadeedi, Akram

An extensive study has been performed to provide a better understanding of the operation principles of doped organic field-effect transistors (OFETs), organic p-i-n diodes, Schottky diodes, and organic permeable base transistors (OPBTs). This has been accomplished by a combination of electrical and structural characterization of these devices. The discussion of doped OFETs focuses on the shift of the threshold voltage due to increased doping concentrations and the generation and transport of minority charge carriers. Doping of pentacene OFETs is achieved by co-evaporation of pentacene with the n-dopant W2(hpp)4. It is found that pentacene thin film are efficiently doped and that a conductivity in the range of 2.6 x 10-6 S cm-1 for 1 wt% to 2.5 x 10-4 S cm-1 for 16 wt% is reached. It is shown that n-doped OFET consisting of an n-doped channel and n-doped contacts are ambipolar. This behavior is surprising, as n-doping the contacts should suppress direct injection of minority charge carriers (holes). It was proposed that minority charge carrier injection and hence the ambipolar characteristic of n-doped OFETs can be explained by Zener tunneling inside the intrinsic pentacene layer underneath the drain electrode. It is shown that the electric field in this layer is indeed in the range of the breakdown field of pentacene based p-i-n Zener homodiodes. Doping the channel has a profound influence on the onset voltage of minority (hole) conduction. The onset voltage can be shifted by lightly n-doping the channel. The shift of onset voltage can be explained by two mechanisms: first, due to a larger voltage that has to be applied to the gate in order to fully deplete the n-doped layer. Second, it can be attributed to an increase in hole trapping by inactive dopants. Moreover, it has been shown that the threshold voltage of majority (electron) conduction is shifted by an increase in the doping concentration, and that the ambipolar OFETs can be turned into unipolar OFETs at high doping concentrations. In subsequent chapters, the working mechanisms of OPBTs are discussed. OPBTs consist of two Schottky diodes (top and bottom diode), and the charge transport in these C60-based Schottky diodes is studied first. Two transport regimes can be distinguished in forward direction - injection limited currents (ILCs) and space charge limited currents (SCLCs). It is found that the current increases exponentially with applied voltage in the ILC regime and depends quadratically on the applied voltage in the SCLC regime. Furthermore, it is observed that the forward and backward currents of the Schottky diode are increased by decreasing the C60 layer thickness, increasing the active area, and increasing the temperature. Furthermore, in order to reach a high performance, various treatments have been applied. Air exposure, a variation of the thickness of the top electrode, as well as annealing of the diodes are used to optimize the diodes. OPBTs are processed by using the semiconductor C60 due its high charge carrier mobility and good film-forming properties. Again, the working mechanism of OPBTs is studied by electrical characterization (base-sweep measurements and output characteristics). To achieve a high performance of OPBTs, various treatments and techniques have been applied. The annealing of the OPBTs after fabrication changes the morphology of the base electrode. Thus, openings (pinholes) are formed in the base electrode, which enables a high current transfer from the upper to lower semiconductor layer. The formation of openings is proved by analyzing SEM and TEM image of the base electrode. Adding a doped layer at the emitter is another process to optimize the OPBTs. The doped layer ensures a high charge carrier injection at the emitter, leading to a high transmission and current gain. Furthermore, it has been observed that the ON/OFF ratio and transconductance of OPBTs increases by decreasing their active area. A very high transconductance gm of 37 S/cm2 is reached, which has the potential to boost the switching speed of organic transistors to 5 MHz. Furthermore, it is shown that the base electrode thickness is an essential parameter for OPBTs. The current gain beta decreases by increasing thickness of base electrode, whereas the ON/OFF ratio increases for thicker base electrodes.

Photochemical Dynamics of Intramolecular Singlet Fission

NASA Astrophysics Data System (ADS)

Lin, Zhou; Iwasaki, Hikari; Van Voorhis, Troy

2017-06-01

Singlet fission (SF) converts a singlet exciton (S_1) into a pair of triplet ones (T_1) via a ``multi-exciton'' (ME) intermediate: S_1 \\longleftrightarrow ^1ME \\longleftrightarrow ^1(T_1T_1) \\longrightarrow 2T_1. In exothermic cases, e.g., crystalline pentacene or its derivatives, the quantum yield of SF can reach 200%. With SF doubling the electric current generated by an incident high-energy photon, the solar conversion efficiency in pentacene-based organic photovoltaics (OPVs) can exceed the Shockley-Queisser limit of 33.7%. The ME state is popularly considered to be a dimeric state with significant charge transfer (CT) character that is strongly coupled to both S_1 and ^1(T_1T_1), while this local model lacks strong support from full quantum dynamics studies. Intramolecular SF (ISF) occurring to covalently-bound dimers in the solution phase is an excellent model for a straightforward dynamics simulation of local excitons. In the present study, we investigate the ISF mechanisms for three covalently-bound dimers of pentacene derivatives, including ortho-, meta-, and para-bis(6,13-bis(triisopropylsilylethynyl)pentacene)benzene, in non-protic solvents. Specifically, we propagate the real-time, non-adiabatic quantum mechanical/molecular mechanical (QM/MM) dynamics on the potential energy surfaces associated with the states of S_1, ^1(T_1T_1) and CT. We explore how the energies of these ISF-relevant states and the non-adiabatic couplings between each other fluctuate with time and the instantaneous molecular configuration (e.g., intermonomer distance and orientation). We also quantitatively compare Condon and non-Condon ISF dynamics with solution-phase spectroscopic data. Our results allow us to understand the roles of CT energy levels in the ISF mechanism and propose a design strategy to maximize ISF efficiency. M. B. Smith and J. Michl, Chem. Rev. 110, 6891 (2010). W. Shockley and H. J. Queisser, J. Appl. Phys. 32, 510 (1961). T. C. Berkelbach, M. S. Hybertsen, and D. R. Reichman, J. Chem. Phys. 141, 074705 (2014). M. G. Mavros, D. Hait, and T. A. Van Voorhis, J. Chem. Phys. 145, 214105 (2016). V. Vaissier, and T. A. Van Voorhis, in preparation.

Characterization of structural and electrostatic complexity in pentacene thin films by scanning probe microscopy

NASA Astrophysics Data System (ADS)

Puntambekar, Kanan Prakash

The advancement of organic electronics for applications in solar energy conversion, printed circuitry, displays, and solid-state lighting depends upon optimization of structure and properties for a variety of organic semiconductor interfaces. Organic semiconductor/insulator (O/I) and organic-metal (O/M) interfaces, in particular, are critical to the operation of organic thin film transistors (OTFTs) currently being developed for printed flexible electronics. Scanning probe microscopy (SPM) is a powerful tool to isolate and characterize the bottlenecks to charge transport at these interfaces. This thesis establishes a direct correlation between the structural disorder and electrical complexity at these interfaces, using various SPM based methods and discusses the implications of such complexity on device performance. To examine the O/M interfaces, surface potentials of operating pentacene TFTs with two different contact geometries (bottom or top) were mapped by Kelvin probe force microscopy (KFM). The surface potential distribution was used to isolate the potential drops at the source and drain contacts. Simultaneously obtained topography and surface potential maps elucidated the correlation between the morphology and contact resistance at the O/M interface; the bottom contact TFTs were observed to be contact limited at large gate voltages, while the top contact TFTs were not contact limited. A direct correlation between structural defects and electric potential variations at the pentacene and silicon dioxide, a common insulator, is demonstrated. Lateral force microscopy (LFM) generates striking images of the polycrystalline microstructure of a monolayer thick pentacene film, allowing clear visualization of the grain boundary network. Further more, surface potential wells localized at the grain boundaries were observed by KFM, suggesting that the grain boundaries may serve as charge carrier (hole) traps. Line dislocations were also revealed in the second monolayer by chemical etching and SPM and produce strong variations in the surface potential that must affect the interfacial charge conductance. Structural disorder at the O/I and O/M interfaces degrades both injection and transport of charge, and therefore needs to be minimized. Thus both visualization and correlation of structural and electrical complexity at these interfaces have important implications for understanding electrical transport in OTFTs and for defining strategies to improve device performance.

Distribution of Localized States from Fine Analysis of Electron Spin Resonance Spectra in Organic Transistors

NASA Astrophysics Data System (ADS)

Matsui, Hiroyuki; Mishchenko, Andrei S.; Hasegawa, Tatsuo

2010-02-01

We developed a novel method for obtaining the distribution of trapped carriers over their degree of localization in organic transistors, based on the fine analysis of electron spin resonance spectra at low enough temperatures where all carriers are localized. To apply the method to pentacene thin-film transistors, we proved through continuous wave saturation experiments that all carriers are localized at below 50 K. We analyzed the spectra at 20 K and found that the major groups of traps comprise localized states having wave functions spanning around 1.5 and 5 molecules and a continuous distribution of states with spatial extent in the range between 6 and 20 molecules.

Distribution of localized states from fine analysis of electron spin resonance spectra in organic transistors.

PubMed

Matsui, Hiroyuki; Mishchenko, Andrei S; Hasegawa, Tatsuo

2010-02-05

We developed a novel method for obtaining the distribution of trapped carriers over their degree of localization in organic transistors, based on the fine analysis of electron spin resonance spectra at low enough temperatures where all carriers are localized. To apply the method to pentacene thin-film transistors, we proved through continuous wave saturation experiments that all carriers are localized at below 50 K. We analyzed the spectra at 20 K and found that the major groups of traps comprise localized states having wave functions spanning around 1.5 and 5 molecules and a continuous distribution of states with spatial extent in the range between 6 and 20 molecules.

Temperature dependence of frequency response characteristics in organic field-effect transistors

NASA Astrophysics Data System (ADS)

Lu, Xubing; Minari, Takeo; Liu, Chuan; Kumatani, Akichika; Liu, J.-M.; Tsukagoshi, Kazuhito

2012-04-01

The frequency response characteristics of semiconductor devices play an essential role in the high-speed operation of electronic devices. We investigated the temperature dependence of dynamic characteristics in pentacene-based organic field-effect transistors and metal-insulator-semiconductor capacitors. As the temperature decreased, the capacitance-voltage characteristics showed large frequency dispersion and a negative shift in the flat-band voltage at high frequencies. The cutoff frequency shows Arrhenius-type temperature dependence with different activation energy values for various gate voltages. These phenomena demonstrate the effects of charge trapping on the frequency response characteristics, since decreased mobility prevents a fast charge response for alternating current signals at low temperatures.

Hopping and band mobilities of pentacene, rubrene, and 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT) from first principle calculations.

PubMed

Kobayashi, Hajime; Kobayashi, Norihito; Hosoi, Shizuka; Koshitani, Naoki; Murakami, Daisuke; Shirasawa, Raku; Kudo, Yoshihiro; Hobara, Daisuke; Tokita, Yuichi; Itabashi, Masao

2013-07-07

Hopping and band mobilities of holes in organic semiconductors at room temperature were estimated from first principle calculations. Relaxation times of charge carriers were evaluated using the acoustic deformation potential model. It is found that van der Waals interactions play an important role in determining accurate relaxation times. The hopping mobilities of pentacene, rubrene, and 2,7-dioctyl[1]benzothieno[3,2-b][1]benzothiophene (C8-BTBT) in bulk single crystalline structures were found to be smaller than 4 cm(2)∕Vs, whereas the band mobilities were estimated between 36 and 58 cm(2)∕Vs, which are close to the maximum reported experimental values. This strongly suggests that band conductivity is dominant in these materials even at room temperature.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Basel, Bettina S.; Zirzlmeier, Johannes; Hetzer, Constantin

When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron–hole pairs, leading to a predicted B50% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state thatmore » precedes formation of the pentacene triplet excitons. In conclusion, using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.« less

Origin of bias-stress induced instability in organic thin-film transistors with semiconducting small-molecule/insulating polymer blend channel.

PubMed

Park, Ji Hoon; Lee, Young Tack; Lee, Hee Sung; Lee, Jun Young; Lee, Kimoon; Lee, Gyu Baek; Han, Jiwon; Kim, Tae Woong; Im, Seongil

2013-03-13

The stabilities of a blending type organic thin-film transistor with phase-separated TIPS-pentacene channel layer were characterized under the conditions of negative-bias-stress (NBS) and positive-bias-stress (PBS). During NBS, threshold voltage (Vth) shifts noticeably. NBS-imposed devices revealed interfacial trap density-of-states (DOS) at 1.56 and 1.66 eV, whereas initial device showed the DOS at only 1.56 eV, as measured by photoexcited charge-collection spectroscopy (PECCS) method. Possible origin of this newly created defect is related to ester group in PMMA, which induces some hole traps at the TIPS-pentacene/i-PMMA interface. PBS-imposed device showed little Vth shift but visible off-current increase as "back-channel" effect, which is attributed to the water molecules trapped on the TFT surface.

Field-modulation spectroscopy of pentacene thin films using field-effect devices: Reconsideration of the excitonic structure

NASA Astrophysics Data System (ADS)

Haas, Simon; Matsui, Hiroyuki; Hasegawa, Tatsuo

2010-10-01

We report pure electric-field effects on the excitonic absorbance of pentacene thin films as measured by unipolar field-effect devices that allowed us to separate the charge accumulation effects. The field-modulated spectra between 1.8 and 2.6 eV can be well fitted with the first derivative curve of Frenkel exciton absorption and its vibronic progression, and at higher energy a field-induced feature appears at around 2.95 eV. The results are in sharp contrast to the electroabsorption spectra reported by Sebastian in previous studies [Chem. Phys. 61, 125 (1981)10.1016/0301-0104(81)85055-0], and leads us to reconsider the excitonic structure including the location of charge-transfer excitons. Nonlinear π -electronic response is discussed based on second-order electro-optic (Kerr) spectra.

Defect healing at room temperature in pentacene thin films and improved transistor performance

NASA Astrophysics Data System (ADS)

Kalb, Wolfgang L.; Meier, Fabian; Mattenberger, Kurt; Batlogg, Bertram

2007-11-01

We report on a healing of defects at room temperature in the organic semiconductor pentacene. This peculiar effect is a direct consequence of the weak intermolecular interaction which is characteristic of organic semiconductors. Pentacene thin-film transistors were fabricated and characterized by in situ gated four-terminal measurements. Under high vacuum conditions (base pressure of order 10-8mbar ), the device performance is found to improve with time. The effective field-effect mobility increases by as much as a factor of 2 and mobilities up to 0.45cm2/Vs were achieved. In addition, the contact resistance decreases by more than an order of magnitude and there is a significant reduction in current hysteresis. Oxygen and nitrogen exposure as well as annealing experiments show the improvement of the electronic parameters to be driven by a thermally promoted process and not by chemical doping. In order to extract the spectral density of trap states from the transistor characteristics, we have implemented a powerful scheme which allows for a calculation of the trap densities with high accuracy in a straightforward fashion. We show the performance improvement to be due to a reduction in the density of shallow traps ⩽0.15eV from the valence band edge, while the energetically deeper traps are essentially unaffected. This work contributes to an understanding of the shallow traps in organic semiconductors and identifies structural point defects within the grains of the polycrystalline thin films as a major cause.

Understanding polymorphism in organic semiconductor thin films through nanoconfinement.

PubMed

Diao, Ying; Lenn, Kristina M; Lee, Wen-Ya; Blood-Forsythe, Martin A; Xu, Jie; Mao, Yisha; Kim, Yeongin; Reinspach, Julia A; Park, Steve; Aspuru-Guzik, Alán; Xue, Gi; Clancy, Paulette; Bao, Zhenan; Mannsfeld, Stefan C B

2014-12-10

Understanding crystal polymorphism is a long-standing challenge relevant to many fields, such as pharmaceuticals, organic semiconductors, pigments, food, and explosives. Controlling polymorphism of organic semiconductors (OSCs) in thin films is particularly important given that such films form the active layer in most organic electronics devices and that dramatic changes in the electronic properties can be induced even by small changes in the molecular packing. However, there are very few polymorphic OSCs for which the structure-property relationships have been elucidated so far. The major challenges lie in the transient nature of metastable forms and the preparation of phase-pure, highly crystalline thin films for resolving the crystal structures and evaluating the charge transport properties. Here we demonstrate that the nanoconfinement effect combined with the flow-enhanced crystal engineering technique is a powerful and likely material-agnostic method to identify existing polymorphs in OSC materials and to prepare the individual pure forms in thin films at ambient conditions. With this method we prepared high quality crystal polymorphs and resolved crystal structures of 6,13-bis(triisopropylsilylethynyl)pentacene (TIPS-pentacene), including a new polymorph discovered via in situ grazing incidence X-ray diffraction and confirmed by molecular mechanic simulations. We further correlated molecular packing with charge transport properties using quantum chemical calculations and charge carrier mobility measurements. In addition, we applied our methodology to a [1]benzothieno[3,2-b][1]1benzothiophene (BTBT) derivative and successfully stabilized its metastable form.

The converse approach to NMR chemical shifts from first-principles: application to finite and infinite aromatic compounds

NASA Astrophysics Data System (ADS)

Thonhauser, T.; Ceresoli, D.; Marzari, N.

2009-03-01

We present first-principles, density-functional theory calculations of the NMR chemical shifts for polycyclic aromatic hydrocarbons, starting with benzene and increasing sizes up to the one- and two-dimensional infinite limits of graphene ribbons and sheets. Our calculations are performed using a combination of the recently developed theory of orbital magnetization in solids, and a novel approach to NMR calculations where chemical shifts are obtained from the derivative of the orbital magnetization with respect to a microscopic, localized magnetic dipole. Using these methods we study on equal footing the ^1H and ^13C shifts in benzene, pyrene, coronene, in naphthalene, anthracene, naphthacene, and pentacene, and finally in graphene, graphite, and an infinite graphene ribbon. Our results show very good agreement with experiments and allow us to characterize the trends for the chemical shifts as a function of system size.

Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Vogiatzis, Konstantinos D.; Ma, Dongxia; Olsen, Jeppe

A new large-scale parallel multiconfigurational self-consistent field (MCSCF) implementation in the open-source NWChem computational chemistry code is presented. The generalized active space approach is used to partition large configuration interaction (CI) vectors and generate a sufficient number of batches that can be distributed to the available cores. Massively parallel CI calculations with large active spaces can be performed. The new parallel MCSCF implementation is tested for the chromium trimer and for an active space of 20 electrons in 20 orbitals, which can now routinely be performed. Unprecedented CI calculations with an active space of 22 electrons in 22 orbitals formore » the pentacene systems were performed and a single CI iteration calculation with an active space of 24 electrons in 24 orbitals for the chromium tetramer was possible. In conclusion, the chromium tetramer corresponds to a CI expansion of one trillion Slater determinants (914 058 513 424) and is the largest conventional CI calculation attempted up to date.« less

Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations

DOE PAGES

Vogiatzis, Konstantinos D.; Ma, Dongxia; Olsen, Jeppe; ...

2017-11-14

A new large-scale parallel multiconfigurational self-consistent field (MCSCF) implementation in the open-source NWChem computational chemistry code is presented. The generalized active space approach is used to partition large configuration interaction (CI) vectors and generate a sufficient number of batches that can be distributed to the available cores. Massively parallel CI calculations with large active spaces can be performed. The new parallel MCSCF implementation is tested for the chromium trimer and for an active space of 20 electrons in 20 orbitals, which can now routinely be performed. Unprecedented CI calculations with an active space of 22 electrons in 22 orbitals formore » the pentacene systems were performed and a single CI iteration calculation with an active space of 24 electrons in 24 orbitals for the chromium tetramer was possible. In conclusion, the chromium tetramer corresponds to a CI expansion of one trillion Slater determinants (914 058 513 424) and is the largest conventional CI calculation attempted up to date.« less

Pushing configuration-interaction to the limit: Towards massively parallel MCSCF calculations

NASA Astrophysics Data System (ADS)

Vogiatzis, Konstantinos D.; Ma, Dongxia; Olsen, Jeppe; Gagliardi, Laura; de Jong, Wibe A.

2017-11-01

A new large-scale parallel multiconfigurational self-consistent field (MCSCF) implementation in the open-source NWChem computational chemistry code is presented. The generalized active space approach is used to partition large configuration interaction (CI) vectors and generate a sufficient number of batches that can be distributed to the available cores. Massively parallel CI calculations with large active spaces can be performed. The new parallel MCSCF implementation is tested for the chromium trimer and for an active space of 20 electrons in 20 orbitals, which can now routinely be performed. Unprecedented CI calculations with an active space of 22 electrons in 22 orbitals for the pentacene systems were performed and a single CI iteration calculation with an active space of 24 electrons in 24 orbitals for the chromium tetramer was possible. The chromium tetramer corresponds to a CI expansion of one trillion Slater determinants (914 058 513 424) and is the largest conventional CI calculation attempted up to date.

Singlet-to-triplet intermediates and triplet exciton dynamics in pentacene thinfilms

NASA Astrophysics Data System (ADS)

Thorsmolle, Verner; Korber, Michael; Obergfell, Emanuel; Kuhlman, Thomas; Campbell, Ian; Crone, Brian; Taylor, Antoinette; Averitt, Richard; Demsar, Jure

Singlet-to-triplet fission in organic semiconductors is a spin-conserving multiexciton process in which one spin-zero singlet excitation is converted into two spin-one triplet excitations on an ultrafast timescale. Current scientific interest into this carrier multiplication process is largely driven by prospects of enhancing the efficiency in photovoltaic applications by generating two long-lived triplet excitons by one photon. The fission process is known to involve intermediate states, known as correlated triplet pairs, with an overall singlet character, before being interchanged into uncorrelated triplets. Here we use broadband femtosecond real-time spectroscopy to study the excited state dynamics in pentacene thin films, elucidating the fission process and the role of intermediate triplet states. VKT and AJT acknowledge support by the LDRD program at Los Alamos National Laboratory and the Department of Energy, Grant No. DE-FG02-04ER118. MK, MO and JD acknowledge support by the Alexander von Humboldt Foundation.

Enhanced magnetic Purcell effect in room-temperature masers

PubMed Central

Breeze, Jonathan; Tan, Ke-Jie; Richards, Benjamin; Sathian, Juna; Oxborrow, Mark; Alford, Neil McN

2015-01-01

Recently, the world’s first room-temperature maser was demonstrated. The maser consisted of a sapphire ring housing a crystal of pentacene-doped p-terphenyl, pumped by a pulsed rhodamine-dye laser. Stimulated emission of microwaves was aided by the high quality factor and small magnetic mode volume of the maser cavity yet the peak optical pumping power was 1.4 kW. Here we report dramatic miniaturization and 2 orders of magnitude reduction in optical pumping power for a room-temperature maser by coupling a strontium titanate resonator with the spin-polarized population inversion provided by triplet states in an optically excited pentacene-doped p-terphenyl crystal. We observe maser emission in a thimble-sized resonator using a xenon flash lamp as an optical pump source with peak optical power of 70 W. This is a significant step towards the goal of continuous maser operation. PMID:25698634

Nucleation of Organic Molecules via a Hot Precursor State: Pentacene on Amorphous Mica

PubMed Central

2013-01-01

Organic thin films have attracted considerable interest due to their applicability in organic electronics. The classical scenario for thin film nucleation is the diffusion-limited aggregation (DLA). Recently, it has been shown that organic thin film growth is better described by attachment-limited aggregation (ALA). However, in both cases, an unusual relationship between the island density and the substrate temperature was observed. Here, we present an aggregation model that goes beyond the classical DLA or ALA models to explain this behavior. We propose that the (hot) molecules impinging on the surface cannot immediately equilibrate to the substrate temperature but remain in a hot precursor state. In this state, the molecules can migrate considerable distances before attaching to a stable or unstable island. This results in a significantly smaller island density than expected by assuming fast equilibration and random diffusion. We have applied our model to pentacene film growth on amorphous Muscovite mica. PMID:24340130

Molecular microelectrostatic view on electronic states near pentacene grain boundaries

NASA Astrophysics Data System (ADS)

Verlaak, Stijn; Heremans, Paul

2007-03-01

Grain boundaries are the most inevitable and pronounced structural defects in pentacene films. To study the effect of those structural defects on the electronic state distribution, the energy levels of a hole on molecules at and near the defect have been calculated using a submolecular self-consistent-polarization-field approach in combination with atomic charge-quadrupole interaction energy calculations. This method has been benchmarked prior to application on four idealized grain boundaries: a grain boundary void, a void with molecules squeezed in between two grains, a boundary between two grains with different crystallographic orientations, and a grain boundary void in which a permanent dipole (e.g., a water molecule) has nested. While idealized, those views highlight different aspects of real grain boundaries. Implications on macroscopic charge transport models are discussed, as well as some relation between growth conditions and the formation of the grain boundary.

Interaction of charge carriers with lattice and molecular phonons in crystalline pentacene

NASA Astrophysics Data System (ADS)

Girlando, Alberto; Grisanti, Luca; Masino, Matteo; Brillante, Aldo; Della Valle, Raffaele G.; Venuti, Elisabetta

2011-08-01

The computational protocol we have developed for the calculation of local (Holstein) and non-local (Peierls) carrier-phonon coupling in molecular organic semiconductors is applied to both the low temperature and high temperature bulk crystalline phases of pentacene. The electronic structure is calculated by the semimpirical INDO/S (Intermediate Neglect of Differential Overlap with Spectroscopic parametrization) method. In the phonon description, the rigid molecule approximation is removed, allowing mixing of low-frequency intra-molecular modes with inter-molecular (lattice) phonons. A clear distinction remains between the low-frequency phonons, which essentially modulate the transfer integral from a molecule to another (Peierls coupling), and the high-frequency intra-molecular phonons, which modulate the on-site energy (Holstein coupling). The results of calculation agree well with the values extracted from experiment. The comparison with similar calculations made for rubrene allows us to discuss the implications for the current models of mobility.

Carrier Propagation Dependence on Applied Potentials in Pentacene Organic Field Effect Transistors Investigated by Impedance Spectroscopy and Electrical Time-of-Flight Techniques

NASA Astrophysics Data System (ADS)

Lin, Jack; Weis, Martin; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2011-04-01

Transient measurements of impedance spectroscopy and electrical time-of-flight (TOF) techniques were used for the evaluation of carrier propagation dependence on applied potentials in a pentacene organic field effect transistor (OFET). These techniques are based on carrier propagation, thus isolates the effect of charge density. The intrinsic mobility which is free from contact resistance effects was obtained by measurement of various channel lengths. The obtained intrinsic mobility shows good correspondence with steady-state current-voltage measurement's saturation mobility. However, their power law relations on mobility vs applied potential resulted in different exponents, suggesting different carrier propagation mechanisms, which is attributable to filling of traps or space charge field in the channel region. The hypothesis was verified by a modified electrical TOF experiment which demonstrated how the accumulated charges in the channel influence the effective mobility.

Concentration-dependent photophysical switching in mixed self-assembled monolayers of pentacene and perylenediimide on gold nanoclusters.

PubMed

Kato, Daiki; Sakai, Hayato; Araki, Yasuyuki; Wada, Takehiko; Tkachenko, Nikolai V; Hasobe, Taku

2018-03-28

Photophysical control and switching on organic-inorganic hybrid interfaces are of great interest in diverse fundamental and applicative research areas. 6,13-Bis(triisopropylsilylethynyl)pentacene (TP) is well-known to exhibit efficient singlet fission (SF) for generation of high-yield triplet excited states in aggregated forms, whereas perylenediimide (PDI) ensembles show the characteristic excimer formation. Additionally, a combination of pentacene (electron donor: D) and PDI (electron acceptor: A) is expected to undergo an efficient photoinduced electron transfer (PET), and absorption of two chromophores combined covers the entire visible region. Therefore, the concentration-dependent mixed self-assembled monolayers (SAMs) composed of two chromophores enable us to control and switch the photophysical processes on a surface. In this work, a series of mixed SAMs composed of TP and PDI units on gold nanoclusters (GNCs) were newly synthesized by changing the relative molecular concentration ratios. Structural control of mixed SAMs on a gold surface based on the concentration ratios was successfully achieved. Time-resolved femtosecond and nanosecond transient absorption measurements clearly demonstrate photophysical control and switching of the above competitive reactions such as SF, electron transfer (ET) and excimer formation. The maximum quantum yields of triplet states (ΦT = ∼170%) and electron transfer (ΦET = ∼95%) were quantitatively evaluated by changing the concentration ratios. The rate constants of SF and excimer processes are largely dependent on the concentration ratios, whereas the rate constants of ET processes approximately remain constant. These findings are also discussed based on the statistical framework of the assembly of chromophores on the gold surface.

Surface Polarity and Self-Structured Nanogrooves Collaboratively Oriented Molecular Packing for High Crystallinity toward Efficient Charge Transport.

PubMed

Ji, Deyang; Xu, Xiaomin; Jiang, Longfeng; Amirjalayer, Saeed; Jiang, Lang; Zhen, Yonggang; Zou, Ye; Yao, Yifan; Dong, Huanli; Yu, Junsheng; Fuchs, Harald; Hu, Wenping

2017-02-22

Efficient charge transport in organic semiconductors is essential for construction of high performance optoelectronic devices. Herein, for the first time, we demonstrate that poly(amic acid) (PAA), a facilely deposited and annealing-free dielectric layer, can tailor the growth of organic semiconductor films with large area and high crystallinity toward efficient charge transport and high mobility in their thin film transistors. Pentacene is used as a model system to demonstrate the concept with mobility up to 30.6 cm 2 V -1 s -1 , comparable to its high quality single crystal devices. The structure of PAA has corrugations with OH groups pointing out of the surface, and the presence of an amide bond further allows adjacent polymer strands to interact via hydrogen bonding, leading to a self-rippled surface perpendicular to the corrugation. On the other hand, the strong polar groups (-COOH/-CONH) of PAA could provide repulsive forces between PAA and pentacene, which results in the vertical orientation of pentacene on the dielectric surface. Indeed, in comparison with its imidized counterpart polyimide (PI), PAA dielectric significantly enhances the film crystallinity, drastically increases the domain size, and decreases the interface trap density, giving rise to superior device performance with high mobility. This concept can be extended to more organic semiconducting systems, e.g., 2,6-diphenylanthracene (DPA), tetracene, copper phthalocyanine (CuPc), and copper hexadecafluorophthalocyanine (F 16 CuPc), demonstrating the general applicability. The results show the importance of combining surface nanogrooves with the strong polarity in orienting the molecular arrangement for high crystallinity toward efficient charge transport in organic semiconductors.

Determination of trap distributions from current characteristics of pentacene field-effect transistors with surface modified gate oxide

NASA Astrophysics Data System (ADS)

Scheinert, Susanne; Pernstich, Kurt P.; Batlogg, Bertram; Paasch, Gernot

2007-11-01

It has been demonstrated [K. P. Pernstich, S. Haas, D. Oberhoff, C. Goldmann, D. J. Gundlach, B. Batlogg, A. N. Rashid, and G. Schitter, J. Appl. Phys. 96, 6431 (2004)] that a controllable shift of the threshold voltage in pentacene thin film transistors is caused by the use of organosilanes with different functional groups forming a self-assembled monolayer (SAM) on the gate oxide. The observed broadening of the subthreshold region indicates that the SAM creates additional trap states. Indeed, it is well known that traps strongly influence the behavior of organic field-effect transistors (OFETs). Therefore, the so-called "amorphous silicon (a-Si) model" has been suggested to be an appropriate model to describe OFETs. The main specifics of this model are transport of carriers above a mobility edge obeying Boltzmann statistics and exponentially distributed tail states and deep trap states. Here, approximate trap distributions are determined by adjusting two-dimensional numerical simulations to the experimental data. It follows from a systematic variation of parameters describing the trap distributions that the existence of both donorlike and acceptorlike trap distributions near the valence band, respectively, and a fixed negative interface charge have to be assumed. For two typical devices with different organosilanes the electrical characteristics can be described well with a donorlike bulk trap distribution, an acceptorlike interface distribution, and/or a fixed negative interface charge. As expected, the density of the fixed or trapped interface charge depends strongly on the surface treatment of the dielectric. There are some limitations in determining the trap distributions caused by either slow time-dependent processes resulting in differences between transfer and output characteristics, or in the uncertainty of the effective mobility.

Dynamics of Large Molecules and Molecular Clusters.

DTIC Science & Technology

1984-06-01

Spectroscop., The high local densities attained in the pexpasion are beneficial for two-photon spectroscopy. High-resolution vibrational two-photon...i.e., anthracene, tetracene and pentacene , in large clusters of Ar, which were synthesized in high-flow supersonic jets (stagnation pressure p : 3000

Reducing the contact resistance in bottom-contact-type organic field-effect transitors using an AgO x interface layer

NASA Astrophysics Data System (ADS)

Minagawa, Masahiro; Kim, Yeongin; Claus, Martin; Bao, Zhenan

2017-09-01

Bottom-contact organic field-effect transistors (OFETs) are prepared by inserting an AgO x layer between a pentacene layer and the source-drain electrodes. The contact resistance in the device is ˜8.1 kΩ·cm with an AgO x layer oxidized for 60 s but reaches 116.9 kΩ·cm with a non-oxidized Ag electrode. The drain current and mobility in the OFETs with the AgO x layer increase with the oxidization time and then gradually plateau, and this trend strongly depends on the work function of the Ag surface. Further, the hole injection is enhanced by the presence of Ag2O but inhibited by the presence of AgO.

Comparison of localized basis and plane-wave basis for density-functional calculations of organic molecules on metals

NASA Astrophysics Data System (ADS)

Lee, Kyuho; Yu, Jaejun; Morikawa, Yoshitada

2007-01-01

Localized pseudoatomic orbitals (PAOs) are mainly optimized and tested for the strong chemical bonds within molecules and solids with their proven accuracy and efficiency, but are prone to significant basis set superposition error (BSSE) for weakly interacting systems. Here we test the accuracy of PAO basis in comparison with the BSSE-free plane-wave basis for the physisorption of pentacene molecule on Au (001) by calculating the binding energy, adsorption height, and energy level alignment. We show that both the large cutoff radius for localized PAOs and the counter-poise correction for BSSE are necessary to obtain well-converged physical properties. Thereby obtained results are as accurate as the plane-wave basis results. The comparison with experiment is given as well.

Transparent ambipolar organic thin film transistors based on multilayer transparent source-drain electrodes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Nan; Hu, Yongsheng, E-mail: huyongsheng@ciomp.ac.cn, E-mail: liuxy@ciomp.ac.cn; Lin, Jie

A fabrication method for transparent ambipolar organic thin film transistors with transparent Sb{sub 2}O{sub 3}/Ag/Sb{sub 2}O{sub 3} (SAS) source and drain electrodes has been developed. A pentacene/N,N′-ditridecylperylene-3,4,9,10-tetracarboxylic di-imide (PTCDI-C13) bilayer heterojunction is used as the active semiconductor. The electrodes are deposited by room temperature electron beam evaporation. The devices are fabricated without damaging the active layers. The SAS electrodes have high transmittance (82.5%) and low sheet resistance (8 Ω/sq). High performance devices with hole and electron mobilities of 0.3 cm{sup 2}/V s and 0.027 cm{sup 2}/V s, respectively, and average visible range transmittance of 72% were obtained. These transistors have potential for transparent logicmore » integrated circuit applications.« less

Polariton-Assisted Singlet Fission in Acene Aggregates.

PubMed

Martínez-Martínez, Luis A; Du, Matthew; F Ribeiro, Raphael; Kéna-Cohen, Stéphane; Yuen-Zhou, Joel

2018-04-19

Singlet fission is an important candidate to increase energy conversion efficiency in organic photovoltaics by providing a pathway to increase the quantum yield of excitons per photon absorbed in select materials. We investigate the dependence of exciton quantum yield for acenes in the strong light-matter interaction (polariton) regime, where the materials are embedded in optical microcavities. Starting from an open-quantum-systems approach, we build a kinetic model for time-evolution of species of interest in the presence of singlet quenchers and show that polaritons can decrease or increase exciton quantum yields compared to the cavity-free case. In particular, we find that hexacene, under the conditions of our model, can feature a higher yield than cavity-free pentacene when assisted by polaritonic effects. Similarly, we show that pentacene yield can be increased when assisted by polariton states. Finally, we address how various relaxation processes between bright and dark states in lossy microcavities affect polariton photochemistry. Our results also provide insights on how to choose microcavities to enhance similarly related chemical processes.

Low-voltage organic strain sensor on plastic using polymer/high- K inorganic hybrid gate dielectrics

NASA Astrophysics Data System (ADS)

Jung, Soyoun; Ji, Taeksoo; Varadan, Vijay K.

2007-12-01

In this paper, gate-induced pentacene semiconductor strain sensors based on hybrid-gate dielectrics using poly-vinylphenol (PVP) and high-K inorganic, Ta IIO 5 are fabricated on flexible substrates, polyethylene naphthalate (PEN). The Ta IIO 5 gate dielectric layer is combined with a thin PVP layer to obtain very smooth and hydrophobic surfaces which improve the molecular structures of pentacene films. The PVP-Ta IIO 5 hybrid-gate dielectric films exhibit a high dielectric capacitance and low leakage current. The sensors adopting thin film transistor (TFT)-like structures show a significantly reduced operating voltage (~6V), and good device characteristics with a field-effect mobility of 1.89 cm2/V•s, a threshold voltage of -0.5 V, and an on/off ratio of 10 3. The strain sensor, one of the practical applications in large-area organic electronics, was characterized with different bending radii of 50, 40, 30, and 20 mm. The sensor output signals were significantly improved with low-operating voltages.

A Direct Mechanism of Ultrafast Intramolecular Singlet Fission in Pentacene Dimers

DOE PAGES

Fuemmeler, Eric G.; Sanders, Samuel N.; Pun, Andrew B.; ...

2016-05-05

Interest in materials that undergo singlet fission (SF) has been catalyzed by the potential to exceed the Shockley–Queisser limit of solar power conversion efficiency. In conventional materials, the mechanism of SF is an intermolecular process (xSF), which is mediated by charge transfer (CT) states and depends sensitively on crystal packing or molecular collisions. In contrast, recently reported covalently coupled pentacenes yield ~2 triplets per photon absorbed in individual molecules: the hallmark of intramolecular singlet fission (iSF). But, the mechanism of iSF is unclear. Here, using multireference electronic structure calculations and transient absorption spectroscopy, we establish that iSF can occur viamore » a direct coupling mechanism that is independent of CT states. Moreover, we show that a near-degeneracy in electronic state energies induced by vibronic coupling to intramolecular modes of the covalent dimer allows for strong mixing between the correlated triplet pair state and the local excitonic state, despite weak direct coupling.« less

Observation of turnover of spontaneous polarization in ferroelectric layer of pentacene/poly-(vinylidene-trifluoroethylene) double-layer capacitor under photo illumination by optical second-harmonic generation measurement

NASA Astrophysics Data System (ADS)

Shi, Zhemin; Taguchi, Dai; Manaka, Takaaki; Iwamoto, Mitsumasa

2016-04-01

The details of turnover process of spontaneous polarization and associated carrier motions in indium-tin oxide/poly-(vinylidene-trifluoroethylene)/pentacene/Au capacitor were analyzed by coupling displacement current measurement (DCM) and electric-field-induced optical second-harmonic generation (EFISHG) measurement. A model was set up from DCM results to depict the relationship between electric field in semiconductor layer and applied external voltage, proving that photo illumination effect on the spontaneous polarization process lied in variation of semiconductor conductivity. The EFISHG measurement directly and selectively probed the electric field distribution in semiconductor layer, modifying the model and revealing detailed carrier behaviors involving photo illumination effect, dipole reversal, and interfacial charging in the device. A further decrease of DCM current in the low voltage region under illumination was found as the result of illumination effect, and the result was argued based on the changing of the total capacitance of the double-layer capacitors.

Ultrafast dynamics of exciton fission in polycrystalline pentacene.

PubMed

Wilson, Mark W B; Rao, Akshay; Clark, Jenny; Kumar, R Sai Santosh; Brida, Daniele; Cerullo, Giulio; Friend, Richard H

2011-08-10

We use ultrafast transient absorption spectroscopy with sub-20 fs time resolution and broad spectral coverage to directly probe the process of exciton fission in polycrystalline thin films of pentacene. We observe that the overwhelming majority of initially photogenerated singlet excitons evolve into triplet excitons on an ∼80 fs time scale independent of the excitation wavelength. This implies that exciton fission occurs at a rate comparable to phonon-mediated exciton localization processes and may proceed directly from the initial, delocalized, state. The singlet population is identified due to the brief presence of stimulated emission, which is emitted at wavelengths which vary with the photon energy of the excitation pulse, a violation of Kasha's Rule that confirms that the lowest-lying singlet state is extremely short-lived. This direct demonstration that triplet generation is both rapid and efficient establishes multiple exciton generation by exciton fission as an attractive route to increased efficiency in organic solar cells. © 2011 American Chemical Society

Electron-flux infrared response to varying π-bond topology in charged aromatic monomers

PubMed Central

Álvaro Galué, Héctor; Oomens, Jos; Buma, Wybren Jan; Redlich, Britta

2016-01-01

The interaction of delocalized π-electrons with molecular vibrations is key to charge transport processes in π-conjugated organic materials based on aromatic monomers. Yet the role that specific aromatic motifs play on charge transfer is poorly understood. Here we show that the molecular edge topology in charged catacondensed aromatic hydrocarbons influences the Herzberg-Teller coupling of π-electrons with molecular vibrations. To this end, we probe the radical cations of picene and pentacene with benchmark armchair- and zigzag-edges using infrared multiple-photon dissociation action spectroscopy and interpret the recorded spectra via quantum-chemical calculations. We demonstrate that infrared bands preserve information on the dipolar π-electron-flux mode enhancement, which is governed by the dynamical evolution of vibronically mixed and correlated one-electron configuration states. Our results reveal that in picene a stronger charge π-flux is generated than in pentacene, which could justify the differences of electronic properties of armchair- versus zigzag-type families of technologically relevant organic molecules. PMID:27577323

Exploring the Influence of Dynamic Disorder on Excitons in Solid Pentacene

NASA Astrophysics Data System (ADS)

Wang, Zhiping; Sharifzadeh, Sahar; Doak, Peter; Lu, Zhenfei; Neaton, Jeffrey

2014-03-01

A complete understanding of the spectroscopic and charge transport properties of organic semiconductors requires knowledge of the role of thermal fluctuations and dynamic disorder. We present a first-principles theoretical study aimed at understanding the degree to which dynamic disorder at room temperature results in energy level broadening and excited-state localization within bulk crystalline pentacene. Ab initio molecular dynamics simulations are well-equilibrated for 7-9 ps and tens of thousands of structural snapshots, taken at 0.5 fs intervals, provide input for many-body perturbation theory within the GW approximation and Bethe-Salpeter equation (BSE) approach. The GW-corrected density of states, including thousands of snapshots, indicates that thermal fluctuations significantly broaden the valence and conduction states by >0.2 eV. Additionally, we investigate the nature and energy of the lowest energy singlet and triplet excitons, computed for a set of uncorrelated and energetically preferred structures. This work supported by DOE; computational resources provided by NERSC.

Core-shell photoabsorption and photoelectron spectra of gas-phase pentacene: experiment and theory.

PubMed

Alagia, Michele; Baldacchini, Chiara; Betti, Maria Grazia; Bussolotti, Fabio; Carravetta, Vincenzo; Ekström, Ulf; Mariani, Carlo; Stranges, Stefano

2005-03-22

The C K-edge photoabsorption and 1s core-level photoemission of pentacene (C22H14) free molecules are experimentally measured, and calculated by self-consistent-field and static-exchange approximation ab initio methods. Six nonequivalent C atoms present in the molecule contribute to the C 1s photoemission spectrum. The complex near-edge structures of the carbon K-edge absorption spectrum present two main groups of discrete transitions between 283 and 288 eV photon energy, due to absorption to pi* virtual orbitals, and broader structures at higher energy, involving sigma* virtual orbitals. The sharp absorption structures to the pi* empty orbitals lay well below the thresholds for the C 1s ionizations, caused by strong excitonic and localization effects. We can definitely explain the C K-edge absorption spectrum as due to both final (virtual) and initial (core) orbital effects, mainly involving excitations to the two lowest-unoccupied molecular orbitals of pi* symmetry, from the six chemically shifted C 1s core orbitals.

Synthesis and photophysical properties of a single bond linked tetracene dimer

NASA Astrophysics Data System (ADS)

Sun, Tingting; Shen, Li; Liu, Heyuan; Sun, Xuan; Li, Xiyou

2016-07-01

A tetracene dimer linked directly by a single bond has been successfully prepared by using electron withdrawing groups to improve the stability. The molecular structure of this dimer is characterized by 1H NMR, MALDI-TOF mass spectroscopy, and elemental analysis. The minimized molecular structure and X-ray crystallography reveal that the tetracene subunits of this dimer adopt an orthogonal configuration. Its absorption spectrum differs significantly from that of its monomeric counterpart, suggesting the presence of strong interactions between the two tetracene subunits. The excited state of this dimer is delocalized on both two tetracene subunits, which is significantly different from that of orthogonal anthracene dimers, but similar with that observed for orthogonal pentacene dimer. Most of the excited states of this dimer decay by radioactive channels, which is different from the localized twisted charge transfer state (LTCT) channel of anthracene dimers and the singlet fission (SF) channel of pentacene dimers. The results of this research suggest that similar orthogonal configurations caused different propertied for acene dimers with different conjugation length.

Core-shell photoabsorption and photoelectron spectra of gas-phase pentacene: Experiment and theory

NASA Astrophysics Data System (ADS)

Alagia, Michele; Baldacchini, Chiara; Betti, Maria Grazia; Bussolotti, Fabio; Carravetta, Vincenzo; Ekström, Ulf; Mariani, Carlo; Stranges, Stefano

2005-03-01

The C K-edge photoabsorption and 1s core-level photoemission of pentacene (C22H14) free molecules are experimentally measured, and calculated by self-consistent-field and static-exchange approximation ab initio methods. Six nonequivalent C atoms present in the molecule contribute to the C 1s photoemission spectrum. The complex near-edge structures of the carbon K-edge absorption spectrum present two main groups of discrete transitions between 283 and 288eV photon energy, due to absorption to π* virtual orbitals, and broader structures at higher energy, involving σ* virtual orbitals. The sharp absorption structures to the π* empty orbitals lay well below the thresholds for the C 1s ionizations, caused by strong excitonic and localization effects. We can definitely explain the C K-edge absorption spectrum as due to both final (virtual) and initial (core) orbital effects, mainly involving excitations to the two lowest-unoccupied molecular orbitals of π* symmetry, from the six chemically shifted C 1s core orbitals.

Vapor-phase-processed fluorinated self-assembled monolayer for organic thin-film transistors

NASA Astrophysics Data System (ADS)

Roh, Jeongkyun; Lee, Changhee; Kwak, Jeonghun; Jung, Byung Jun; Kim, Hyeok

2015-09-01

A vapor-phase-processed fluorinated silazane self-assembled monolayer (SAM), 1,3-bis(trifluoropropyl)-1,1,3,3-tetramethyldisilazane (FPDS), was introduced as a surface modifier for pentacene-based organic thin-film transistors (OTFTs). A remarkable improvement in the field effect mobility from 0.25 cm2/Vs (without SAM-treatment) to 0.42 cm2/Vs (with FPDS-treatment) was observed, which was attributed to the better pentacene growth on a hydrophobic surface. A significant reduction in the contact resistance was also observed by FPDS treatment due to the improved bulk conductivity and diminished charge trapping at the gate dielectric surface by the SAM treatment. In addition, FPDS treatment efficiently improved the bias stability of the OTFTs; the drain-to-source current degradation by the bias stress was greatly reduced from 80% to 50% by FPDS treatment, and the characteristic time for charge trapping of the FPDS treated OTFTs was approximately one order of magnitude larger than that of the OTFTs without SAM treatment.

Direct X-ray photoconversion in flexible organic thin film devices operated below 1 V

PubMed Central

Basiricò, Laura; Ciavatti, Andrea; Cramer, Tobias; Cosseddu, Piero; Bonfiglio, Annalisa; Fraboni, Beatrice

2016-01-01

The application of organic electronic materials for the detection of ionizing radiations is very appealing thanks to their mechanical flexibility, low-cost and simple processing in comparison to their inorganic counterpart. In this work we investigate the direct X-ray photoconversion process in organic thin film photoconductors. The devices are realized by drop casting solution-processed bis-(triisopropylsilylethynyl)pentacene (TIPS-pentacene) onto flexible plastic substrates patterned with metal electrodes; they exhibit a strong sensitivity to X-rays despite the low X-ray photon absorption typical of low-Z organic materials. We propose a model, based on the accumulation of photogenerated charges and photoconductive gain, able to describe the magnitude as well as the dynamics of the X-ray-induced photocurrent. This finding allows us to fabricate and test a flexible 2 × 2 pixelated X-ray detector operating at 0.2 V, with gain and sensitivity up to 4.7 × 104 and 77,000 nC mGy−1 cm−3, respectively. PMID:27708274

Efficient Syntheses of Novel Fluoro-Substituted Pentacenes and Azapentacenes: Molecular and Solid-State Properties.

PubMed

Schwaben, Jonas; Münster, Niels; Klues, Michael; Breuer, Tobias; Hofmann, Philipp; Harms, Klaus; Witte, Gregor; Koert, Ulrich

2015-09-21

Non-symmetrical 6,13-disubstituted pentacenes bearing trifluoromethyl and aryl substituents have been synthesized starting from pentacenequinone. Diazapentacenes with a variety of fluorine substituents were prepared either via a Hartwig-Buchwald aryl amination route or by a SNAr strategy. As a result of a non-symmetric substitution pattern containing electron-donating substituents in combination with electron-accepting fluorine substituents, the synthesized compounds feature distinct molecular dipoles. All compounds are analyzed regarding their optoelectronic properties in solution with special focus on the frontier orbital energies as well as their molecular packing in the crystal structures. The analyses of isolated molecules are complemented by thin-film studies to examine their solid-state properties. A precise comparison between these and the molecular properties gave detailed insights into the exciton binding energies of these compounds, which are explained by means of a simple model considering the molecular packing and polarizabilities. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Light sensing in a photoresponsive, organic-based complementary inverter.

PubMed

Kim, Sungyoung; Lim, Taehoon; Sim, Kyoseung; Kim, Hyojoong; Choi, Youngill; Park, Keechan; Pyo, Seungmoon

2011-05-01

A photoresponsive organic complementary inverter was fabricated and its light sensing characteristics was studied. An organic circuit was fabricated by integrating p-channel pentacene and n-channel copper hexadecafluorophthalocyanine (F16CuPc) organic thin-film transistors (OTFTs) with a polymeric gate dielectric. The F16CuPc OTFT showed typical n-type characteristics and a strong photoresponse under illumination. Whereas under illumination, the pentacene OTFT showed a relatively weak photoresponse with typical p-type characteristics. The characteristics of the organic electro-optical circuit could be controlled by the incident light intensity, a gate bias, or both. The logic threshold (V(M), when V(IN) = V(OUT)) was reduced from 28.6 V without illumination to 19.9 V at 6.94 mW/cm². By using solely optical or a combination of optical and electrical pulse signals, light sensing was demonstrated in this type of organic circuit, suggesting that the circuit can be potentially used in various optoelectronic applications, including optical sensors, photodetectors and electro-optical transceivers.

Photoconductivity in organic thin films: From picoseconds to seconds after excitation

NASA Astrophysics Data System (ADS)

Day, J.; Subramanian, S.; Anthony, J. E.; Lu, Z.; Twieg, R. J.; Ostroverkhova, O.

2008-06-01

We present a detailed study, on time scales from picoseconds to seconds, of transient and continuous wave (cw) photoconductivity in solution-grown thin films of functionalized pentacene (Pc), anthradithiophene (ADT), and dicyanomethylenedihydrofuran (DCDHF). In all films, at temperatures of 285-350 K, we observe fast carrier photogeneration and nonthermally activated charge transport on picosecond time scales. At ˜30 ps after photoexcitation at room temperature and at applied electric field of 1.2×104 V/cm, values obtained for the product of mobility and photogeneration efficiency, μη, in ADT-tri-isoproplysilylethynyl-(TIPS)-F, Pc-TIPS, and DCDHF films are ˜0.018-0.025, ˜0.01-0.022, and ˜0.002-0.004 cm2/V s, respectively, depending on the film quality, and are weakly electric field dependent. In functionalized ADT and Pc films, the power-law decay dynamics of the transient photoconductivity is observed, on time scales of up to ˜1 μs after photoexcitation, in the best samples. In contrast, in DCDHF amorphous glass, most of the photogenerated carriers are trapped within ˜200 ps. Transport of photoexcited carriers on longer time scales is probed by cw illumination through an optical chopper, with a variable chopper frequency. In contrast with what is observed on picosecond time scales, charge carriers on millisecond and longer time scales are predominantly localized, and are characterized by a broad distribution of carrier lifetimes. Such carriers make the principal contributions to dc photoconductivity.

Physical implication of transition voltage in organic nano-floating-gate nonvolatile memories

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Shun; Gao, Xu, E-mail: wangsd@suda.edu.cn, E-mail: gaoxu@suda.edu.cn; Zhong, Ya-Nan

High-performance pentacene-based organic field-effect transistor nonvolatile memories, using polystyrene as a tunneling dielectric and Au nanoparticles as a nano-floating-gate, show parallelogram-like transfer characteristics with a featured transition point. The transition voltage at the transition point corresponds to a threshold electric field in the tunneling dielectric, over which stored electrons in the nano-floating-gate will start to leak out. The transition voltage can be modulated depending on the bias configuration and device structure. For p-type active layers, optimized transition voltage should be on the negative side of but close to the reading voltage, which can simultaneously achieve a high ON/OFF ratio andmore » good memory retention.« less

Imaging the wave functions of adsorbed molecules

PubMed Central

Lüftner, Daniel; Ules, Thomas; Reinisch, Eva Maria; Koller, Georg; Soubatch, Serguei; Tautz, F. Stefan; Ramsey, Michael G.; Puschnig, Peter

2014-01-01

The basis for a quantum-mechanical description of matter is electron wave functions. For atoms and molecules, their spatial distributions and phases are known as orbitals. Although orbitals are very powerful concepts, experimentally only the electron densities and -energy levels are directly observable. Regardless whether orbitals are observed in real space with scanning probe experiments, or in reciprocal space by photoemission, the phase information of the orbital is lost. Here, we show that the experimental momentum maps of angle-resolved photoemission from molecular orbitals can be transformed to real-space orbitals via an iterative procedure which also retrieves the lost phase information. This is demonstrated with images obtained of a number of orbitals of the molecules pentacene (C22H14) and perylene-3,4,9,10-tetracarboxylic dianhydride (C24H8O6), adsorbed on silver, which are in excellent agreement with ab initio calculations. The procedure requires no a priori knowledge of the orbitals and is shown to be simple and robust. PMID:24344291

Fluorescence Excitation of Single Molecules,

DTIC Science & Technology

localized neighborhoods and to optical addressing of local spots in solids may now be envisioned. The purpose of this presentation is to show that single...molecules can be studied at helium temperatures by means of a fairly simple setup, at least in the very favorable case of pentacene in terphenyl

Probe-based measurement of lateral single-electron transfer between individual molecules

PubMed Central

Steurer, Wolfram; Fatayer, Shadi; Gross, Leo; Meyer, Gerhard

2015-01-01

The field of molecular electronics aims at using single molecules as functional building blocks for electronics components, such as switches, rectifiers or transistors. A key challenge is to perform measurements with atomistic control over the alignment of the molecule and its contacting electrodes. Here we use atomic force microscopy to examine charge transfer between weakly coupled pentacene molecules on insulating films with single-electron sensitivity and control over the atomistic details. We show that, in addition to the imaging capability, the probe tip can be used to control the charge state of individual molecules and to detect charge transfers to/from the tip, as well as between individual molecules. Our approach represents a novel route for molecular charge transfer studies with a host of opportunities, especially in combination with single atom/molecule manipulation and nanopatterning techniques. PMID:26387533