Charge transport in columnar stacked triphenylenes: Effects of conformational fluctuations on charge transfer integrals and site energies

Transfer integrals for oligos with different bases have been calculated using INDO/Koopman's approximation to unveil the charge transport mechanism in DNA. The sequences, G(A) n G , n = 1, 2, …, 10; G(A) x G(A) y G , x + y = 9; and G(A) x G(A) y G(A) z G , x + y + z = 8, were employed to interpret the Guanine (G) and Adenine(A) hopping. Adenine hopping is found to be faster in G(A) n G sequences with longer Adenine bridges (n ≥ 3). Inserting G-bases in between G(A) 10 G led to a decrease in the value of transfer integrals. Close analysis has revealed that bridge closer to 3′-end forms a hopping bottleneck; however, the presence of bridge at 5′-end enhances the charge transfer through A-hopping. Further insertion of single G sites in G(A) x G(A) y G (where x + y = 9) reduces the transfer integrals, thus explaining the hampering of A-hopping. Hence, sequences of the type G(A) n G , n > 3, are better suited for their application as molecular wire. Finally, studies on the effect of flipping of bases, i.e. flipping G:C to C:G on transfer integrals, have revealed that helical distortions and conformational changes due to sequence variations lead to changes in coupling, which is highly unpredictable.

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Suppression of dynamic disorder by electrostatic interactions in structurally close organic semiconductors

Physical Chemistry Chemical Physics ◽

10.1039/d1cp01599k ◽

2021 ◽

Author(s):

Andrey Yurievich Sosorev ◽

Olga Parashchuk ◽

Nikita Tukachev ◽

Dmitry Maslennikov ◽

Dmitry Dominsky ◽

...

Keyword(s):

Charge Transfer ◽

Charge Transport ◽

Organic Semiconductors ◽

Electrostatic Interactions ◽

High Mobility ◽

Dynamic Disorder ◽

Transfer Integrals

Dynamic disorder manifested in fluctuations of charge transfer integrals considerably hinders charge transport in high-mobility organic semiconductors. Accordingly, strategies for suppression of the dynamic disorder are highly desirable. In this...

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Electronic Structure, Electron-Phonon Coupling and Charge Transport in Crystalline Rubrene Under Mechanical Strain

10.26434/chemrxiv.8015645 ◽

2019 ◽

Author(s):

Michael Ruggiero ◽

Sergio Ciuchi ◽

Simone Fratini ◽

Gabriele D'Avino

Keyword(s):

Charge Transfer ◽

Charge Transport ◽

Mechanical Response ◽

Compressive Strain ◽

Mechanical Strain ◽

High Mobility ◽

Phonon Coupling ◽

Electron Phonon Coupling ◽

Transfer Integrals ◽

Energetic Disorder

<div> <div> <div><p>Motivated by the potential for application of organic semiconductors in exible electronics, we present a theoretical study aiming at elucidating the interplay between mechanical strain and electronic, vibrational and charge transport properties of the prototypical high-mobility molecular semiconductor rubrene. Our study considers several factors that can play a role in the electro-mechanical response of a soft, van-der-Waals bonded, molecular crystal, such as intermolecular charge transfer integrals, lattice dynamics and electron phonon coupling. We find that compressive strain leads to an increase in magnitude of charge transfer integrals but also of the energetic disorder hampering the mobility. Charge transport simulations, based on the transient localization framework and fed with first-principles inputs, reveal a remarkably different response to strain applied along different crystal axes, in line with most recent experiments. The critical interplay between energetic disorder of intrinsic and extrinsic nature on the mobility-strain relationship is also discussed. The theoretical approach proposed in this work paves the way for the systematic study of the electro-mechanical response of different classes of high-mobility molecular semiconductors.</p></div> </div> </div>

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Electronic Structure, Electron-Phonon Coupling and Charge Transport in Crystalline Rubrene Under Mechanical Strain

10.26434/chemrxiv.8015645.v1 ◽

2019 ◽

Author(s):

Michael Ruggiero ◽

Sergio Ciuchi ◽

Simone Fratini ◽

Gabriele D'Avino

Keyword(s):

Charge Transfer ◽

Charge Transport ◽

Mechanical Response ◽

Compressive Strain ◽

Mechanical Strain ◽

High Mobility ◽

Phonon Coupling ◽

Electron Phonon Coupling ◽

Transfer Integrals ◽

Energetic Disorder

<div> <div> <div><p>Motivated by the potential for application of organic semiconductors in exible electronics, we present a theoretical study aiming at elucidating the interplay between mechanical strain and electronic, vibrational and charge transport properties of the prototypical high-mobility molecular semiconductor rubrene. Our study considers several factors that can play a role in the electro-mechanical response of a soft, van-der-Waals bonded, molecular crystal, such as intermolecular charge transfer integrals, lattice dynamics and electron phonon coupling. We find that compressive strain leads to an increase in magnitude of charge transfer integrals but also of the energetic disorder hampering the mobility. Charge transport simulations, based on the transient localization framework and fed with first-principles inputs, reveal a remarkably different response to strain applied along different crystal axes, in line with most recent experiments. The critical interplay between energetic disorder of intrinsic and extrinsic nature on the mobility-strain relationship is also discussed. The theoretical approach proposed in this work paves the way for the systematic study of the electro-mechanical response of different classes of high-mobility molecular semiconductors.</p></div> </div> </div>

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Growth direction dependent separate-channel charge transport in organic weak charge-transfer co-crystal of anthracene-DTTCNQ

Materials Horizons ◽

10.1039/d1mh01767e ◽

2022 ◽

Author(s):

Hui Jiang ◽

Jun Ye ◽

Peng Hu ◽

Shengli Zhu ◽

Yanqin Liang ◽

...

Keyword(s):

Charge Transfer ◽

Charge Transport ◽

Electronic Properties ◽

Single Crystals ◽

Organic Semiconductors ◽

Crystal Engineering ◽

Molecular Crystal ◽

Growth Direction ◽

Weak Charge ◽

Separate Channel

Co-crystallization is an efficient way of molecular crystal engineering to tune the electronic properties of organic semiconductors. In this work, we synthesized anthracene-4,8-bis(dicyanomethylene)4,8-dihydrobenzo[1,2-b:4,5-b’]-dithiophene (DTTCNQ) single crystals as a template to...

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Intermolecular Charge-Transfer-Induced Strong Optical Emission from Herringbone H-Aggregates

10.26434/chemrxiv.14484462.v1 ◽

2021 ◽

Author(s):

Qi Sun ◽

Jiajun Ren ◽

Tong Jiang ◽

Qian Peng ◽

Qi Ou ◽

...

Keyword(s):

Charge Transfer ◽

Optical Emission ◽

Light Emitting ◽

High Charge ◽

Organic Light ◽

Intermolecular Charge Transfer ◽

Transfer Integrals ◽

Strong Luminescence ◽

Theoretical Finding ◽

Three State Model

Superior organic light-emitting transistors (OLETs) materials require two conventionally exclusive properties: strong luminescence and high charge mobilities. We propose a three-state model through localized diabatization to quantitative analyze excited state structures for various herringbone (HB) H-aggregates and demonstrate that for some investigated systems, the low-lying intermolecular charge-transfer (CT) state couples with the bright Frenkel exciton (FE) and forms a dipole-allowed S<sub>1</sub> that lies below the dark state, proceeding strong luminescence. Specifically, such conversion in luminescence properties occurs when the electron- and hole-transfer integrals ( and ) are of the same sign and is notably larger than the excitonic coupling (<i>J</i>), i.e., . This theoretical finding can not only explain and rationalize recent experimental results on DPA and dNaAnt, both with OLET property, but also unravel an exciting scenario where strong luminescence and high charge mobilities are compatible, which will considerably broaden the aperture of novel OLET design.

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Molecular dynamics and charge transport in organic semiconductors: a classical approach to modeling electron transfer

Chemical Science ◽

10.1039/c6sc04547b ◽

2017 ◽

Vol 8 (4) ◽

pp. 2597-2609 ◽

Cited By ~ 10

Author(s):

Kenley M. Pelzer ◽

Álvaro Vázquez-Mayagoitia ◽

Laura E. Ratcliff ◽

Sergei Tretiak ◽

Raymond A. Bair ◽

...

Keyword(s):

Molecular Dynamics ◽

Electron Transfer ◽

Charge Transfer ◽

Charge Transport ◽

Ab Initio ◽

Organic Semiconductors ◽

Multiscale Approach ◽

Classical Approach ◽

Classical Molecular Dynamics

Using ab initio calculations of charges in PCBM fullerenes, a multiscale approach applies classical molecular dynamics to model charge transfer.

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The role of charge transfer at reduced graphene oxide/organic semiconductor interface on the charge transport properties

Organic Electronics ◽

10.1016/j.orgel.2019.105499 ◽

2020 ◽

Vol 77 ◽

pp. 105499 ◽

Cited By ~ 2

Author(s):

Srinivasa Rao Pathipati ◽

Egon Pavlica ◽

Emanuele Treossi ◽

Vincenzo Palermo ◽

Gvido Bratina

Keyword(s):

Graphene Oxide ◽

Charge Transfer ◽

Charge Transport ◽

Transport Properties ◽

Reduced Graphene Oxide ◽

Organic Semiconductor ◽

Semiconductor Interface ◽

Reduced Graphene

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Charge transport properties of co-evaporated organic–inorganic thin film charge transfer complexes: effects of intermolecular interactions

Journal of Materials Chemistry C ◽

10.1039/d0tc04278a ◽

2020 ◽

Vol 8 (47) ◽

pp. 16725-16729

Author(s):

Dong Shen ◽

Yan Wu ◽

Ming-Fai Lo ◽

Chun-Sing Lee

Keyword(s):

Thin Film ◽

Charge Transfer ◽

Charge Transport ◽

Transport Properties ◽

Intermolecular Interactions ◽

Charge Transfer Complexes

Charge transport properties of the organic–inorganic MoO3 : 6T CTC thin film can be dramatically tuned via rubbing. The effects of intermolecular interactions on these changes are studied in detail.

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