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The role of local potential minima on charge transport in thin organic semiconductor layers
Egon Pavlica, Raveendra Babu Penumala, Bratina Gvido, 2016, izvirni znanstveni članek

Opis: We have performed a systematic study of dependence of time-resolved photocurrent on the point of charge excitation within the organic semiconductor channel formed by two coplanar metal electrodes. The results confirm that spatial variation of electric field between the electrodes crucially determines transport of photogenerated charge carriers through the organic layer. Time-of-flight measurements of photocurrent demonstrate that the transit time of photogenerated charge carrier packets drifting between the two electrodes decreases with increasing travelling distance. Such counterintuitive result cannot be reconciled with the spatial distribution of electric field between coplanar electrodes, alone. It is also in contrast to expected role of space-charge screening of external electric field. Supported by Monte Carlo simulations of hopping transport in disordered organic semiconductor layer, we submit that the space-charge screens the external electric field and captures slower charge carriers from the photogenerated charge carrier packet. The remaining faster carriers, exhibit velocity distribution with significantly higher mean value and shorter transit time.
Najdeno v: ključnih besedah
Povzetek najdenega: ...Charge transport, Organic semiconductors, Time of flight, Mobility, Traps...
Ključne besede: Charge transport, Organic semiconductors, Time of flight, Mobility, Traps
Objavljeno: 23.12.2016; Ogledov: 4291; Prenosov: 0
.pdf Polno besedilo (950,46 KB)

Nadiia Pastukhova, 2018, doktorska disertacija

Opis: In this work, we experimentally studied the influence of photoexcitation energy influence on the charge transport in organic semiconductors. Organic semiconductors were small molecules like corannulene, perylene and pentacene derivatives, polymers such as polythiophene and benzothiophene derivatives, and graphene, along with combinations of these materials in heterojunctions or composites. The first part of this study is focused on the photoexcitation energy influence on the transient photoconductivity of non-crystalline curved π-conjugated corannulene layers. The enhanced photoconductivity, in the energy range where optical absorption is absent, is deduced from theoretical predictions of corannulene gas-phase excited state spectra. Theoretical analysis reveals a consistent contribution involving transitions to Super Atomic Molecular Orbitals (SAMOs), a unique set of diffuse orbitals typical of curved π-conjugated molecules. More, the photoconductivity of the curved corannulene was compared to the π-conjugated planar N,N′-1H,1H- perfluorobutyldicyanoperylene-carboxydi-imide (PDIF-CN2), where the photoexcitation energy dependence of photocurrent closely follows the optical absorption spectrum. We next characterized charge transport in poly(3-hexylthiophene) (P3HT) layers deposited from solution. Our results indicate that time-of-flight (TOF) mobility depends on the photoexcitation energy. It is 0.4× 10 −3 cm 2 /Vs at 2.3 eV (530 nm) and doubles at 4.8 eV (260 nm). TOF mobility was compared to field-effect (FET) mobility of P3HT field-effect transistors (OFETs). The FET mobility was similar to the 2.3 eV excitation TOF mobility. In order to improve charge mobility, graphene nanoparticles were blended within a P3HT solution before the deposition. We found that the mobility significantly improves upon the addition of graphene nanoparticles of a weight ratio as low as 0.2 %. FET mobility increases with graphene concentration up to a value of 2.3× 10 −2 cm 2 /Vs at 3.2 %. The results demonstrate that phase segregation starts to influence charge transport at graphene concentration of 0.8 % and above. Hence, the graphene cannot form a bridged conduction channel between electrodes, which would cancel the semiconducting effect of the polymer composite. An alternative approach to enhance mobility is to optimize the molecular ordering of organic semiconductors. For that purpose, we studied an innovative nanomesh device. Free-standing nanomesh devices were used to form nanojunctions of N,N′- iiDioctyl-3,4,9,10-perylenedicarboximide (PTCDI-C8) nanowires and crystalline bis(triisopropylsilylethinyl)pentacene (TIPS-PEN). We characterized the photocurrent response time of this novel nanomesh scaffold device. The photoresponse time depends on the photon energy. It is between 4.5 − 5.6 ns at 500 nm excitation wavelength and between 6.7 − 7.7 ns at 700 nm excitation wavelength. In addition, we found that thermal annealing reduces charge carrier trapping in crystalline nanowires. This confirms that the structural defects are crucial to obtaining high photon-to-charge conversion efficiency and subsequent transport from pn junction in heterostructured materials. Structural defects also influence the power conversion efficiency of organic heterostructured photovoltaics (OPVs). Anticipating that polymers with different backbone lengths produce different level of structural defects, we examined charge transport dependence on the molecular weight of poly[4,8-bis(5-(2- ethylhexyl)thiophen-2-yl)benzo[1,2-b;4,5-b']dithiophene-2,6-diyl-alt-(4-(2- ethylhexyl)-3-fluorothieno[3,4-b]thiophene-)-2-carboxylate-2-6-diyl] (PTB7-Th) from 50 kDa to 300 kDa. We found p-type hopping transport in PTB7-Th, characterized by 0.1 – 3× 10 −2 cm 2 /Vs mobility, which increases with temperature and electric field. The polymer molecular weight exhibits a non-trivial influence on charge transport. FET mobility in the saturation regime increases with molecular weight. A similar trend is observed in TOF mobility and FET mobility in the linear regime, except for the 100kDa polymer, which manifests in the highest mobility due to reduced charge trapping. The lowest trapping at the dielectric interface of OFET is observed at 200 kDa. In addition, the 200 kDa polymer exhibits the lowest activation energy of the charge transport. Although the 100 kDa polymer indicates the highest mobility, OPVs using the 200 kDa polymer exhibit the best performance in terms of power conversion efficiency.
Najdeno v: ključnih besedah
Povzetek najdenega: ...the influence of photoexcitation energy influence on the charge transport in organic semiconductors. Organic semiconductors were small... ...solution. Our results indicate that time-of-flight (TOF) mobility depends on the photoexcitation energy. It is 0.4×...
Ključne besede: organic semiconductors, optical absorption spectroscopy, time-of-flight photoconductivity, transient photocurrent spectroscopy, organic thin film transistors, atomic force microscopy, superatomic molecular orbitals, pn heterojunction, organic nanowires, graphene, composites, charge mobility, charge trapping, temperature dependence, photodetector, photovoltaic, solar cell, organic electronics
Objavljeno: 08.10.2018; Ogledov: 4116; Prenosov: 139
.pdf Polno besedilo (4,56 MB)

Elucidation of Donor:Acceptor Phase Separation in Nonfullerene Organic Solar Cells and Its Implications on Device Performance and Charge Carrier Mobility
Sebastian F. Hoefler, Georg Haberfehlner, Thomas Rath, Andreas Keilbach, Mathias Hobisch, Alexander Dixon, Egon Pavlica, Gvido Bratina, Gerald Kothleitner, Ferdinand Hofer, Gregor Trimmel, 2019, izvirni znanstveni članek

Opis: In bulk-heterojunction solar cells, the device performance strongly depends on the donor and acceptor properties, the phase separation in the absorber layer, and the formation of a bicontinuous network. While this phase separation is well explored for polymer:fullerene solar cells, only little is known for polymer:nonfullerene acceptor solar cells. The main hurdle in this regard is often the chemical similarity of the conjugated polymer donor and the organic nonfullerene acceptor (NFA), which makes the analysis of the phase separation via atomic force microscopic (AFM) phase images or conventional transmission electron microscopy difficult. In this work, we use the donor polymer PTB7-Th and the small molecule acceptor O-IDTBR as the model system and visualized the phase separation in PTB7-Th:O-IDTBR bulk-heterojunctions with different donor:acceptor ratios via scanning transmission electron microscopy (STEM) high-angle annular dark-field (HAADF) images and electron energy loss spectroscopy (EELS) based elemental mapping, which resulted in a good contrast between the donor and the acceptor despite very low differences in the chemical composition. AFM as well as grazing-incidence wide-angle X-ray scattering (GIWAXS) investigations support the electron microscopic data. Furthermore, we elucidate the implications of the phase separation on the device performance as well as charge carrier mobilities in the bulk-heterojunction layers, and a high performance of the solar cells was found over a relatively broad range of polymer domain sizes. This can be related to the larger domain sizes of the acceptor phase with higher amounts of O-IDTBR in the blend, while the polymer donor phase still forms continuous pathways to the electrode, which keeps the hole mobility at a relatively constant level.
Najdeno v: ključnih besedah
Ključne besede: nanomorphology bulk-heterojunction scanning transmission electron microscopy organic photovoltaics charge carrier mobility
Objavljeno: 15.01.2020; Ogledov: 2018; Prenosov: 69
.pdf Polno besedilo (6,22 MB)

A pyrrolopyridazinedione-based copolymer for fullerene-free organic solar cells
Astrid-Caroline Knall, Samuel Rabensteiner, Sebastian F. Hoefler, Matiss Reinfelds, Mathias Hobisch, Heike M. A. Ehmann, Nadiia Pastukhova, Egon Pavlica, Gvido Bratina, Illie Hanzu, Shuguang Wen, Renqiang Yang, Gregor Trimmel, Thomas Rath, 2021, izvirni znanstveni članek

Opis: The recent success of non-fullerene acceptors in organic photovoltaics also entails a change in the requirements to the polymer donor in terms of optical and morphological properties leading to a demand for novel conjugated polymers. Herein, we report on the synthesis of a 1,4-bis-(thiophene-2-yl)-pyrrolopyridazinedione based copolymer with 2-ethylhexyl substituents on the pyrrolopyridazinedione moiety. A 2D conjugated benzodithiophene (BDT) was chosen as comonomer. The resulting copolymer T-EHPPD-T-EHBDT showed a molecular weight of 10.2 kDa, an optical band gap of 1.79 eV, a hole mobility of 1.8 × 10−4 cm2 V−1 s−1 and a preferred face-on orientation with regard to the substrate. The comparably wide band gap as well as the determined energy levels (HOMO: −5.47 eV, LUMO: −3.68 eV) match well with the narrow band gap non-fullerene acceptor ITIC-F, which was used as the acceptor phase in the bulk heterojunction absorber layers in the investigated solar cells. The solar cells, prepared in inverted architecture, revealed power conversion efficiencies up to 7.4% using a donor:acceptor ratio of 1 : 1 in the absorber layer.
Najdeno v: ključnih besedah
Povzetek najdenega: ...non-fullerene solar cells, charge transport, charge mobility, power conversion efficiency...
Ključne besede: non-fullerene solar cells, charge transport, charge mobility, power conversion efficiency
Objavljeno: 27.01.2021; Ogledov: 1526; Prenosov: 0
.pdf Polno besedilo (2,68 MB)

Enhancement of indacenodithiophene–benzothiadiazole copolymer field-effect mobility with MXenes
Hu Chen, Manisha Chhikara, Nadiia Pastukhova, Jurij Urbančič, Iain Mcculloch, Huanhuan Shi, Ali Shaygan Nia, Xinliang Feng, Egon Pavlica, Gvido Bratina, 2022, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: The predominant mode of charge carrier transport in thin layers of organic semiconductors (OSs) is thermally-activated hopping between localized states. This results in lower charge mobility compared to inorganic semiconductors precluding the use of OSs in high-speed electronic devices. Therefore, significant effort is invested to improve charge carrier mobility of OS thin layers, which form the basis of most of the organic electronic devices. Recent advances in the field of two-dimensional (2D) materials stimulated their use as addition to OS thin layers to boost the charge carrier mobility. MXenes promise to deliver most of the benefits of 2D materials coupled with large scale fabrication capability. Herein we examined Ti3C2X (X is O or OH group termination) MXene, as a candidate to improve charge carrier mobility in thin layer of indacenodithiophene-co-benzothiadiazole (IDTBT), a polymer exhibiting high electron mobility in defect-free crystalline layers. In our work we demonstrate that improvement in electron mobility in solution-cast IDTBT thin layers can be achieved by depositing a non-connected network of MXene flakes at the gate-dielectric/IDBT interface. Bottom-gate field-effect transistors (FETs) comprising of Au electrodes on n-doped silicon wafer covered with 230 nm of thermally deposited SiO2 were prepared and characterized. Charge carrier mobilities determined from transfer characteristics of FETs composing neat IDTBT channels were found to be in the range of 1 - 2×10−2 cm2/Vs. Devices comprising MXene flakes at the interface between SiO2 and IDTBT, instead exhibited a factor of four increase in electron mobility, while preserving the on/off ratio of 104.
Najdeno v: ključnih besedah
Povzetek najdenega: ...The predominant mode of charge carrier transport in thin layers of organic...
Ključne besede: MXene, IDTBT, charge carrier mobility, OFET
Objavljeno: 20.10.2022; Ogledov: 144; Prenosov: 2
.pdf Polno besedilo (82,61 KB)
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Photoexcited charge mobility in quasi two-dimensional polyacetylene
Nadiia Pastukhova, Kejun Liu, Renhao Dong, Gvido Bratina, Xinliang Feng, Egon Pavlica, 2022, objavljeni povzetek znanstvenega prispevka na konferenci

Opis: Two-dimensional conjugated polymers (2DCPs) have been described and recognised as crystalline, one- to two-layer polymer nanosheets prepared by 2D covalent polymerization exhibiting strong in-plane π-electron delocalization with two orthogonal directions and weak out-of-plane π-π stacking.[1,2] The extension of polymer dimensionality into two dimensions improves the alignment of individual polymer sheets and overcomes the limitations associated with charge carrier hopping between polymer chains in one-dimensional and crosslinked polymers.[3] Compared to other two-dimensional materials such as graphene or transition metal dichalcogenides, 2DCPs offer a high degree of flexibility in chemical design and are compatible with liquid-based processing methods. Various 2DCPs have been synthesised by surfactant monolayer-assisted interfacial synthesis (SMAIS).[5] Of particular interest is the photoresponse of these materials due to their tunable properties, such as bandgap and associated wavelength-dependent photoexcitation, which enables a wide range of applications in optoelectronic devices. Using time-of-flight photoconductivity (TOF-PC) measurements [4], we investigate the charge transport properties of 2D polyacetylene prepared by SMAIS method. We preform TOF-PC measurement of 2D polyacetylene using a focused nanosecond pulse laser at 325 nm and electrode separation of 250 µm. From the bias polarity and time duration of the photocurrent, we can determine the polarity, velocity and mobility of photoexcited charge carriers as a function of applied bias voltage and excitation wavelength. Using excitation at 325 m, we observed an electron mobility in the range of 150 cm2 V-1 s-1, which is in the realm of most advances small-molecule single-crystal organic semiconductors and almost an order of magnitude higher than linear polymeric semiconductors.
Najdeno v: ključnih besedah
Ključne besede: Two-dimensional conjugated polymers, 2DCPs, 2Dpolymers, charge mobility, time-of-flight photoconductivity
Objavljeno: 29.11.2022; Ogledov: 57; Prenosov: 0
.pdf Polno besedilo (530,29 KB)

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