Exceptional Dewetting of Organic Semiconductor Films: The Case of Dinaphthothienothiophene (DNTT) at Dielectric Interfaces

Breuer, Tobias; Karthäuser, Andrea; Klemm, Hagen W.; Genuzio, Francesca; Peschel, Gina; Fuhrich, Alexander; Schmidt, Thomas; Witte, Gregor

doi:10.1021/acsami.6b15902

Cited by 29 publications

(49 citation statements)

References 67 publications

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“…Therefore, the film structure results from a minimization of the surface free energy of the films which favors the formation of planes where molecules are densely packed, as shown schematically in Figure . This is the (001) surface which exhibits the highest coordination of the DNTT molecules like it is formed on SiO 2 . Interestingly, the work function changes for DNTT monolayers are rather similar in all cases, but are dominated by the choice of the metal substrate.…”

Section: Discussionmentioning

confidence: 92%

“…Finally, we note that controlling the molecular orientation and film structure is decisive for the realization of horizontal as well as vertical OFETs since the highly anisotropic electronic properties of the DNTT films result in strongly different device characteristics for varied orientations. Moreover, the distinct dewetting introduces an additional complication to the realization of devices since the current paths may be interrupted …”

Section: Discussionmentioning

confidence: 99%

“…Despite their structural similarity, both the materials exhibit, however, different growth characteristics. For example, a notable dewetting was found upon growth of DNTT films on SiO 2 and other dielectrics as well as on graphite substrates, while smoother PEN films are formed on these substrates . On the other hand, PEN (as well as many other PAH) films that are deposited onto crystalline metal substrates reveal a distinct dewetting and island formation beyond the first monolayer (ML), which is attributed to the structural misfit between the flat‐lying chemisorbed molecules in the seed layer and the herringbone motif in the bulk crystal structure .…”

Section: Introductionmentioning

confidence: 99%

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Interface Structure and Evolution of Dinaphthothienothiophene (DNTT) Films on Noble Metal Substrates

Dreher

Bischof

Widdascheck

et al. 2018

Adv Materials Inter

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The latter characteristic is particularly important since charge carrier mobility and transport properties of crystalline π-conjugated molecular materials are typically strongly anisotropic, [5] which underlines the importance of a precise structural control of OSC films at the contact interfaces.Among the newly synthesized OSCs, dinaphthothienothiophene (DNTT) has received particular attention because it combines a remarkably high charge carrier mobility [6,7] with distinct chemical robustness, [8,9] hence making it superior to previous OSC benchmark systems based on pentacene (PEN) or rubrene. [10][11][12] DNTT is a planar polycyclic hydrocarbon (PAH) with similar shape and intermolecular interaction as PEN [13] and likewise adopts a layered crystal structure. In the (001) planes, which are the typical surface planes in DNTT crystals, the molecules are uprightly oriented and exhibit a face-on-edge herringbone packing arrangement. [6] Despite their structural similarity, both the materials exhibit, however, different growth characteristics. For example, a notable dewetting was found upon growth of DNTT films on SiO 2 and other dielectrics as well as on graphite substrates, [14] while smoother PEN films are formed on these substrates. [15,16] On the other hand, PEN (as well as many other PAH) films that are deposited onto crystalline metal substrates reveal a distinct dewetting and island formation beyond the first monolayer (ML), [17][18][19] which is attributed to the structural misfit between the flat-lying chemisorbed molecules in the seed layer and the herringbone motif in the bulk crystal structure. [20] Despite their importance for device applications, interfaces between DNTT and metals are hardly studied so far. The only exception is the previous work of Hasegawa et al. who studied the initial stage of DNTT film growth on Au(111) and reported a transition from an initially diluted phase into a densely packed adlayer which comprises a mixture of flat-lying and inclined molecules. [21] While this growth scenario is of particular interest, as it would allow adjusting the interface structure to the crystal bulk phase, no clear evidence for such a tilting was given and also the structure of thicker films was not analyzed. A similar mechanism has been identified before for the growth of PEN Dinaphthothienothiophene (DNTT) is a promising new organic semiconductor which combines high charge carrier mobility with chemical robustness. Although the properties of organic electronic devices are largely determined by the interfaces with electrodes, the interface between DNTT and metals is hardly studied so far. Here, the interface structures of DNTT on Ag(111) and multilayers are examined and they are compared with films grown on polycrystalline and (111) surfaces of silver and gold. In the seedlayer regime, two different interface structures formed by exclusively flatlying molecules and a herringbone arrangement are identified for increased coverages. Combining low energy electron diffraction, scanning tunneling micro...

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Section: Discussionmentioning

confidence: 92%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Interface Structure and Evolution of Dinaphthothienothiophene (DNTT) Films on Noble Metal Substrates

Dreher

Bischof

Widdascheck

et al. 2018

Adv Materials Inter

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“…Detailed interface studies were enabled using highly ordered single crystals as substrates, which were employed to monitor the dynamics of film growth and microscopic diffusion processes as well as post-deposition structural changes. [183,184] Furthermore, pentacene (PEN) and perylene were exploited for excitonic studies of the various crystalline phases, [185,186] with temperature-dependent studies revealing exciton energy shifts as a consequence of strain at interfaces. [187,188] Additionally, individual molecular domains were probed optically for hetero-epitaxial organic films of perfluoropentacene (PFP) on alkali halide substrates.…”

Section: Nanoscale Systems and Characterization Techniquesmentioning

confidence: 99%

Advances in Functional Nanomaterials Science

Rahimi‐Iman

2020

Annalen der Physik

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Technologies employing nanomaterials, such as electronics, optoelectronics, nanobiotechnologies, quantum optics, and nanophotonics, are perceived as the key drivers of investigations on novel and functional materials and their nanostructures for various applications. It is well understood that the study of such materials and structures has been of great importance for the optimization and development of electrical and optical devices. From such devices, one does not only expect higher efficiencies, but also access to the development of completely new concepts, which are strongly demanded by modern information‐processing, quantum, or medical technologies, and sensing applications. In this context, a wide range of aspects such as the physics of novel materials, as well as materials engineering, characterization, and applications are summarized here. Novel materials, which can be used, for instance, for energy harvesting or light generation, as well as for future logic devices; material engineering, which can lead to improved device functionality and performance in optoelectronics; material physics, the study of which allows insight to be gained into optical and electrical properties of nanostructured systems and quantum materials; and technologies/devices, addressing progress on the application side of sophisticated material systems and quantum structures, are highlighted using representative examples.

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“…Recent studies revealed the distinctive structural features of DNTT such as interfacial layer formation and spontaneous molecular rearrangement. [34,35] Such a development underlines that additional verification is required to establish in-depth understanding of this particular semiconductor's morphology.…”

Section: Film Morphologymentioning

confidence: 99%

Potentiometric Parameterization of Dinaphtho[2,3‐b:2′,3′‐f]thieno[3,2‐b]thiophene Field‐Effect Transistors with a Varying Degree of Nonidealities

Kim

Thomas

Kim

et al. 2018

Adv Elect Materials

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in a fully standardized manner with, for instance, no extra light, heat, or active areas involved. [4] By contrast, widely discussed parameters (i.e., charge-carrier mobility and threshold voltage, V T ) for organic field-effect transistors (OFETs) are model parameters, meaning that the numbers are inherently dependent on the model used as well as the procedure followed to implement this model. [5,6] Therefore, the lack of consensus may lead to discrepancies in parameters extracted even from the same current-voltage curve.In 2004, Horowitz et al. summarized and extended a series of their earlier works to clarify nonidealities, or disagreement with metal-oxide-semiconductor field-effect transistors (MOSFETs) in OFET devices. [7] As illustrated here, gate-voltage (V G ) dependence of mobility and existence of the contact resistances (R c ) are two common and theoretically justifiable sources of deviations from ideal MOSFET characteristics. Until recently, many experimental studies employed techniques such as the transmission-line method (TLM) or gated fourpoint probe measurements (gFPP), which can in principle directly probe these phenomena by separating the channel and contact properties. [8][9][10][11][12][13][14] In our view, the reported data bring strong evidence for the pronounced variability in relative strengths, and voltage-or structure dependence of the contact and channel effects, which makes different theoretical frameworks often necessary to understand different devices. Nonetheless, the MOSFET current-voltage model has been employed quite universally for simple parameter extraction. In 2016, Gundlach and co-workers used impedance spectroscopy to systematically address mobility overestimation in rubrene single-crystal transistors, [15] an issue that in fact originates from neglecting R c and/or noncontextually adopting simplified equations. In this context, it is timely to critically reassess basic assumptions of the device parameters, specific behavioral nonidealities, and associated calculation issues. Ideally, growing efforts into such a process will be transformed into carefully thought-out and broadly accepted practices for OFET research.In this article, we report on the use of scanning Kelvin probe microscopy (SKPM) and correlated analysis aimed at generalizable parameterization. SKPM is a powerful, surface-sensitive technique that can directly probe critical resistive pathways in OFETs to quantify material-and interface-related parameters. Furthermore, SKPM holds some advantages over the TLM or gFPP in that neither averaging Taking full account of the contact effects and including an explicit threshold voltage in calculation are shown to be critical to access the intrinsic carrier mobility, while simple derivative-based extraction may over-or underestimate it. Further analytical developments correlate individual physical parameters, leading to the discovery that pentafluorobenzenethiol self-assembled on gold predominantly affects the carrier mobility rather than the injection barrier.

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Exceptional Dewetting of Organic Semiconductor Films: The Case of Dinaphthothienothiophene (DNTT) at Dielectric Interfaces

Cited by 29 publications

References 67 publications

Interface Structure and Evolution of Dinaphthothienothiophene (DNTT) Films on Noble Metal Substrates

Interface Structure and Evolution of Dinaphthothienothiophene (DNTT) Films on Noble Metal Substrates

Advances in Functional Nanomaterials Science

Potentiometric Parameterization of Dinaphtho[2,3‐b:2′,3′‐f]thieno[3,2‐b]thiophene Field‐Effect Transistors with a Varying Degree of Nonidealities

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