The interplay of interfaces, supramolecular assembly, and electronics in organic semiconductors

Boehm, Belinda; Nguyễn, Hương Thị Lan; Huang, David M.

doi:10.1088/1361-648x/ab2ac2

Cited by 22 publications

(28 citation statements)

References 179 publications

(431 reference statements)

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“…New‐generation OLEDs are produced by vapor deposition (VP) of organic materials that form layers, wherein the molecular orientation is documented to be a key property capable to improve outcoupling and charge transport efficiency. [ 2–10 ]…”

Section: Introductionmentioning

confidence: 99%

Bidimensional H‐Bond Network Promotes Structural Order and Electron Transport in BPyMPMs Molecular Semiconductor

Correa

Giunchi

Muccioli

et al. 2021

Advcd Theory and Sims

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The presence of a hydrogen bond (H‐Bond) network has been proved to impact significantly the efficiency of organic light‐emitting diode (OLED) devices by promoting molecular orientation and structural anisotropy in thin films. The design of specific compounds to control H‐Bond network formation in an amorphous material, and hence to improve OLED performances, is needed. A successful example is given by the bi‐pyridyl‐based family n‐type of organic semiconductors named BPyMPM. The experimental evidences demonstrate a surprisingly higher electron mobility in thin film composed of 4,6‐bis(3,5‐di(pyridine‐4‐yl)phenyl)‐2‐methylpyrimidine (B4PyMPM (B4)), which is almost two order of magnitude higher than mobility measured for very similar member of the family, 4,6‐bis(3,5‐di(pyridine‐2‐yl)phenyl)‐2‐methylpyrimidine (B2PyMPM (B2)). Herein, a comprehensive computational study is presented, wherein classical and ab initio methods are combined, to investigate the 2D H‐Bond network in B4 and B2 thin films. The results indicate that B4 forms a larger number of intermolecular C‐H···N H‐Bonds that promote a higher orientational and positional order in B4 films, and superior electron transport properties.

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Section: Introductionmentioning

confidence: 99%

Bidimensional H‐Bond Network Promotes Structural Order and Electron Transport in BPyMPMs Molecular Semiconductor

Correa

Giunchi

Muccioli

et al. 2021

Advcd Theory and Sims

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“…2,[8][9][10][11][12] However, isotropic CG models may not always provide the most accurate, efficient, or physically transparent CG description of system properties. For molecules consisting of large, rigid, anisotropic fragments, which includes important classes of molecules such as nucleic acids, 13,14 liquid crystals, 15 and organic semiconductors [16][17][18][19][20] (due to their extended π-conjugation), anisotropic-particle CG models can more accurately represent the shape and interaction anisotropy using a smaller number of CG particles. This potentially increases simulation speed compared with the use of isotropic CG particles for a given level of accuracy.…”

Section: Introductionmentioning

confidence: 99%

“…This is the case for organic semiconductors, for which molecu-lar ordering and alignment at the material interfaces play crucial roles in determining the performance of organic electronic devices such as solar cells, light-emitting diodes and transistors. 17,[21][22][23] Implementation of MD simulations of anisotropic CG models is facilitated by well-established analytical non-bonded pair potentials, with the most commonly used being the Gay-Berne 24 and RE-squared 25 potentials for ellipsoidal particles. Advantages of using anisotropic CG models have been demonstrated in recent approaches to simulate organic material systems, [26][27][28][29] in which both large-scale conformational properties and small-scale anisotropic molecular arrangements were obtained.…”

Section: Introductionmentioning

confidence: 99%

Systematic Bottom-Up Molecular Coarse-Graining via Force Matching using Anisotropic Particles

Huang

Nguyễn

2022

Preprint

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We derive a systematic and general method for parametrizing coarse-grained molecular models consisting of anisotropic particles from fine-grained (e.g. all-atom) models for condensed-phase molecular dynamics simulations. The method, which we call anisotropic force-matching coarse-graining (AFM-CG), is based on rigorous statistical mechanical principles, enforcing consistency between the coarse-grained and fine-grained phase-space distributions to derive equations for the coarse-grained forces, masses, and moments of inertia in terms of properties of a condensed-phase fine-grained system. We verify the accuracy and efficiency of the method by coarse-graining liquid-state systems of two different anisotropic organic molecules, benzene and perylene, and show that the parametrized coarse-grained models more accurately describe properties of these systems than previous anisotropic coarse-grained models parametrized using other methods that do not account for finite-temperature and many-body effects on the condensed-phase coarse-grained interactions. The AFM-CG method will be useful for developing accurate and efficient dynamical simulation models of condensed-phase systems of molecules consisting of large, rigid, anisotropic fragments, such as nucleic acids, liquid crystals, and organic semiconductors.

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“…Although the importance of controlling interface orientation in OSC devices is generally well understood, and there is no shortage of experimental [16][17][18]24 or computational [25][26][27][28][29][30] examples of preferential alignment of anisotropic molecules at interfaces, there remain few general rules for predicting alignment at either the solid or vapour interface from the chemical structure of OSC molecules. We have recently extensively reviewed the subject in the context of OSCs, 31 and despite a number of factors being implicated in controlling molecular orientation, in many cases an understanding of the general physical principles that dictate this behaviour was lacking, especially at the solid interface.…”

Section: Introductionmentioning

confidence: 99%

A simple predictor of interface orientation of mesogenic fluids and its implications for organic semiconductors

Boehm

Huang

2022

Preprint

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From classical molecular dynamics simulations, we identify a simple and general predictor of molecular orientation at solid and vapour interfaces of isotropic fluids of anisotropic particles based on their shape and interaction anisotropy. For a wide variety of inter-particle interactions, temperatures, and substrate types within the range of typical organic semiconductors and their processing conditions, we find remarkable universal scaling of the orientation at the interface with the free energy calculated from pair interactions between close-packed nearest neighbours and an empirically derived universal relationship between the entropy and the shape anisotropy and bulk volume fraction of the fluid particles. The face-on orientation of fluid particles at the solid interface is generally predicted to be the equilibrium structure, although the alignment can be controlled by tuning the particle shape and substrate type, while changing the strength of fluid--fluid interactions is likely to play a less effective role. At the vapour interface, only the side-on structure is predicted, and conditions for which the face-on structure may be preferred, such as low temperature, low interaction anisotropy, or low shape anisotropy, are likely to result in little orientation preference (due to the low anisotropy) or be associated with a phase transition to an anisotropic bulk phase for systems with interactions in the range of typical organic semiconductors. Based on these results, we propose a set of guidelines for the rational design and processing of organic semiconductors to achieve a target orientation at a solid or vapour interface.

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The interplay of interfaces, supramolecular assembly, and electronics in organic semiconductors

Cited by 22 publications

References 179 publications

Bidimensional H‐Bond Network Promotes Structural Order and Electron Transport in BPyMPMs Molecular Semiconductor

Bidimensional H‐Bond Network Promotes Structural Order and Electron Transport in BPyMPMs Molecular Semiconductor

Systematic Bottom-Up Molecular Coarse-Graining via Force Matching using Anisotropic Particles

A simple predictor of interface orientation of mesogenic fluids and its implications for organic semiconductors

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