Quantitative Prediction of Anisotropic Carrier Mobilities for BN-Embedded Perylene Diimides in Three-Dimensional Space

Abstract

Herein, we systematically studied the electronic structures and conducting properties of BN-embedded perylene diimides (B2N2-PDIs): 6-CH, 6-EH, and 6-DIPP reported by Wang et al. (J. Am. Chem. Soc. 2022, 144, 3091–3098) and discussed the influences of partially substituting C–C units of the π-electron core with B–N units on the reorganization energies associated with hole-transport (λh) and electron-transport (λe) process, ionization potential, and electron affinity of PDIs. Our calculations revealed that the incorporation of B–N units lowered the λe by 4–9%, while the electron affinity of PDI is almost unaffected. Just as PDIs, B2N2-PDIs have the potential to be developed as high-efficiency n-type organic semiconducting materials. Furthermore, we simulated the three-dimensional angular resolution anisotropic mobility of 6-CH, 6-EH, and 6-DIPP for the first time. It is found that 6-EH and 6-CH exhibit typical n-type charge carrier-transport properties with a mobility of up to 1.45 and 0.31 cm2 V–1 s–1, respectively. The predicted anisotropic mobility range for 6-EH is consistent with the reported mobility in organic field-effect transistor devices. Moreover, 6-DIPP possesses excellent intrinsic hole mobility, and its highest mobility can be reached up to 107 cm2 s–1 V–1 due to the small λh value and strong electronic coupling between substituents of 2,6-diisopropylphenyl.

Three-Dimensional Anisotropic Carrier Mobility and Structure–Property Relationships for [1]Benzothieno[3,2-b][1]benzothiophene Derivatives: A Theoretical Study

“…The intermolecular charge-transfer process in organic semiconducting materials is mainly determined by two parameters: the λ value and the V value. , The λ value can be evaluated through analyzing the contributions from each vibrational mode to the total relaxation energy (NM analysis method), which has been widely used in the calculations of λ λ = prefix∑ λ normali = prefix∑ ( ω i Δ Q i 2 ) / 2 Here, Δ Q i represents the displacement along the normal mode Q i between the equilibrium geometries of the neutral and charged molecules, and ω i is the corresponding frequency.…”

“…The intermolecular charge-transfer process in organic semiconducting materials is mainly determined by two parameters: the λ value and the V value. 17,18 The λ value can be evaluated through analyzing the contributions from each vibrational mode to the total relaxation energy (NM analysis method), which has been widely used in the calculations of λ…”

Double Alkyl Side Chains Functionalized Polyimide as Gate Dielectrics for Application in Organic Transistors

“…Organic thin-film transistors (OTFTs) have attracted wide attention as a constituent of next-generation electronics in the application field of wearable and stretchable devices, nonvolatile memory, sensors, etc. − In recent years, various studies and efforts have been carried out to improve the performance of OTFTs devices by developing high-quality organic semiconductor materials. Compared with organic semiconductor materials, − the gate dielectric layer as an important component of OTFTs is equally important, but the research progress is still lagging behind.…”