TY - JOUR
T1 - Predictive Model of Charge Mobilities in Organic Semiconductor Small Molecules with Force-Matched Potentials
AU - Dantanarayana, Varuni
AU - Nematiaram, Tahereh
AU - Vong, Daniel
AU - Anthony, John E.
AU - Troisi, Alessandro
AU - Nguyen Cong, Kien
AU - Goldman, Nir
AU - Faller, Roland
AU - Moulé, Adam J.
N1 - Publisher Copyright:
Copyright © 2020 American Chemical Society.
PY - 2020/6/9
Y1 - 2020/6/9
N2 - Charge mobility of crystalline organic semiconductors (OSC) is limited by local dynamic disorder. Recently, the charge mobility for several high mobility OSCs, including TIPS-pentacene, were accurately predicted from a density functional theory (DFT) simulation constrained by the crystal structure and the inelastic neutron scattering spectrum, which provide direct measures of the structure and the dynamic disorder in the length scale and energy range of interest. However, the computational expense required for calculating all of the atomic and molecular forces is prohibitive. Here we demonstrate the use of density functional tight binding (DFTB), a semiempirical quantum mechanical method that is 2 to 3 orders of magnitude more efficient than DFT. We show that force matching a many-body interaction potential to DFT derived forces yields highly accurate DFTB models capable of reproducing the low-frequency intricacies of experimental inelastic neutron scattering (INS) spectra and accurately predicting charge mobility. We subsequently predicted charge mobilities from our DFTB model of a number of previously unstudied structural analogues to TIPS-pentacene using dynamic disorder from DFTB and transient localization theory. The approach we establish here could provide a truly rapid simulation pathway for accurate materials properties prediction, in our vision applied to new OSCs with tailored properties.
AB - Charge mobility of crystalline organic semiconductors (OSC) is limited by local dynamic disorder. Recently, the charge mobility for several high mobility OSCs, including TIPS-pentacene, were accurately predicted from a density functional theory (DFT) simulation constrained by the crystal structure and the inelastic neutron scattering spectrum, which provide direct measures of the structure and the dynamic disorder in the length scale and energy range of interest. However, the computational expense required for calculating all of the atomic and molecular forces is prohibitive. Here we demonstrate the use of density functional tight binding (DFTB), a semiempirical quantum mechanical method that is 2 to 3 orders of magnitude more efficient than DFT. We show that force matching a many-body interaction potential to DFT derived forces yields highly accurate DFTB models capable of reproducing the low-frequency intricacies of experimental inelastic neutron scattering (INS) spectra and accurately predicting charge mobility. We subsequently predicted charge mobilities from our DFTB model of a number of previously unstudied structural analogues to TIPS-pentacene using dynamic disorder from DFTB and transient localization theory. The approach we establish here could provide a truly rapid simulation pathway for accurate materials properties prediction, in our vision applied to new OSCs with tailored properties.
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U2 - 10.1021/acs.jctc.0c00211
DO - 10.1021/acs.jctc.0c00211
M3 - Article
C2 - 32401495
AN - SCOPUS:85086281457
SN - 1549-9618
VL - 16
SP - 3494
EP - 3503
JO - Journal of Chemical Theory and Computation
JF - Journal of Chemical Theory and Computation
IS - 6
ER -