Article
Chemistry, Physical
Mojtaba Alipour, Tahereh Izadkhast
Summary: Hyperfluorescence has been introduced as a promising strategy to achieve high color purity and enhanced stability in organic light-emitting diodes (OLEDs). In this study, the alignments of excited-states in fluorescent emitters (FEs) were investigated using optimally tuned range-separated hybrid functionals (OT-RSHs). Several models were proposed and validated to accurately describe the excited-states ordering in hyperfluorescence-based materials. The best-performing model was found to be the OT-RSHs-PCM with the correct asymptotic behavior and no (low) short-range Hartree-Fock exchange contribution. This study provides recommended models for theoretical modeling and confirming experimental observations in the field of hyperfluorescence-based OLEDs.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Bernhard Kretz, David A. Egger
Summary: Accurate non-adiabatic couplings can be calculated using the optimally tuned range-separated hybrid functionals within the framework of linear-response time-dependent density functional theory, providing an efficient alternative to wave-function-based techniques in the modeling of radiationless decay mechanisms in photochemical processes.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Guy Ohad, Dahvyd Wing, Stephen E. Gant, Ayala V. Cohen, Jonah B. Haber, Francisca Sagredo, Marina R. Filip, Jeffrey B. Neaton, Leeor Kronik
Summary: In this study, we applied the Wannier-localized optimally tuned screened range-separated hybrid functional to calculate the band gaps of typical halide perovskites. The results showed that the method performed accurately with satisfyingly small errors compared to experimental data and previous many-body perturbation theory calculations.
PHYSICAL REVIEW MATERIALS
(2022)
Article
Chemistry, Physical
Dan Mao, Xin-Rui Chen, Dong-Heng Li, Xiang-Yang Liu, Ganglong Cui, Laicai Li
Summary: In this study, the ultrafast charge transfer in a nonfullerene all-small-molecule donor-acceptor system was investigated using linear-response time dependent density functional theory (LR-TDDFT)-based nonadiabatic dynamics simulations. The results provide important insights into the molecular structure, energy level positions, and charge transfer processes in the system.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Marvin Friede, Sebastian Ehlert, Stefan Grimme, Jan-Michael Mewes
Summary: This study investigates the interdependency between dispersion correction parameters and the range-separation parameter omega in large molecules. The results show that some functionals are strongly affected by omega values, leading to overbinding and poor performance. Strategies to mitigate these issues are discussed, providing insights for future improvements.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2023)
Article
Chemistry, Multidisciplinary
J. Patrick Zobel, Ayla Kruse, Omar Baig, Stefan Lochbrunner, Sergey I. I. Bokarev, Oliver Kuehn, Leticia Gonzalez, Olga S. S. Bokareva
Summary: This paper investigates the influence of optimally tuned parameters on the excited state dynamics, using the example of the iron complex [Fe(cpmp)(2)](2+) with push-pull ligands. The study finds that different sets of optimal parameters lead to different relaxation pathways and timescales. The set in better agreement with CASPT2 calculations predicts deactivation in the manifold of metal-centered states, in better agreement with the experimental reference data.
Article
Chemistry, Physical
Tahereh Izadkhast, Mojtaba Alipour
Summary: Predicting non-adiabatic couplings is crucial for studying non-radiative processes. The authors developed and validated optimally tuned range-separated hybrid functionals (OT-RSHs) to accurately calculate non-adiabatic couplings and related properties within time-dependent density functional theory. They found that the OT-RSHs based on specific density functional approximations, incorporating short-range Hartree-Fock exchange, performed the best. These OT-RSHs provide computationally efficient alternatives for studying non-adiabatic systems and screening novel candidates prior to synthesis.
JOURNAL OF CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Satter Rohman, Rahul Kar
Summary: In this study, computationally inexpensive, nonempirically tuned functionals (ELF* and Sol*) were used to investigate the properties of five organic molecules used in OSLDs. The results showed that ELF* and Sol* functionals accurately reproduced the emission energies in toluene and CBP film environments, while the IP-tuned functional with excited-state geometry performed better in the gas phase. The study also compared different computational methods and reported oscillator strength values.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Physical
Caroline A. A. McKeon, Samia M. M. Hamed, Fabien Bruneval, Jeffrey B. B. Neaton
Summary: The ab initio GW-BSE approach with optimally tuned range-separated hybrids can suppress starting point dependence for molecules, leading to accuracy similar to higher-order wavefunction-based theories.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Shuai Liu, Sha-Sha Liu, Xiao-Mei Tang, Xiang-Yang Liu, Jia-Jia Yang, Ganglong Cui, Laicai Li
Summary: In this study, the photoinduced dynamics of donor-acceptor dyads formed using zinc phthalocyanine and perylenediimide were investigated using a combination of the OT-SRSH functional, the PCM model, and NAMD simulations. The presence of a solvent was found to significantly influence the excited state dynamics, leading to photoinduced electron transfer.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2023)
Article
Chemistry, Physical
Mojtaba Alipour, Samaneh Damiri
Summary: In this work, the excited-state characteristics of organic semiconductor dyes used in electrically pumped OSLDs were investigated using optimally tuned range-separated hybrids (OT-RSHs). Several variants of OT-RSHs, along with their combination forms, were proposed for reliable prediction of emission energies and oscillator strengths in both the gas and solvent phases. The newly designed OT-RSHs outperformed standard RSHs and other density functionals in describing the excited-state properties of OSLD compounds. The computational cost of the models was also examined.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Materials Science, Multidisciplinary
Shahidul Alam, Vojtech Nadazdy, Tomas Vary, Christian Friebe, Rico Meitzner, Johannes Ahner, Aman Anand, Safakath Karuthedath, Catherine S. P. De Castro, Clemens Gohler, Stefanie Dietz, Jonathan Cann, Christian Kaestner, Alexander Konkin, Wichard Beenken, Arthur Markus Anton, Christoph Ulbricht, Andreas Sperlich, Martin D. Hager, Uwe Ritter, Friedrich Kremer, Oliver Brueggemann, Ulrich S. Schubert, Daniel A. M. Egbe, Gregory C. Welch, Vladimir Dyakonov, Carsten Deibel, Frederic Laquai, Harald Hoppe
Summary: This study highlights the significance of molecular energy level offsets in driving photoinduced charge transfer in organic solar cells. By utilizing energy-resolved electrochemical impedance spectroscopy, various donor-acceptor combinations were analyzed, leading to insights into charge generation mechanisms and factors influencing molecular energy level alignment.
JOURNAL OF MATERIALS CHEMISTRY C
(2021)
Article
Chemistry, Physical
Soumyajit Sarkar
Summary: We quantitatively studied the accuracy of electronic density calculated using the optimally tuned range-separated hybrid (OT-RSH) functional method in this research. The dipole moments of 152 polar molecules were calculated using the OT-RSH functional and compared with literature coupled-cluster calculations. Another test set consisting of 14 closed-shell diatomic molecules was used to evaluate the performance of OT-RSH in predicting electronic densities. The results showed that OT-RSH-derived electronic densities and dipole moments were as accurate as some better performing global hybrid functionals, overcoming the limitations of empirical choices in traditional global hybrid functionals.
THEORETICAL CHEMISTRY ACCOUNTS
(2023)
Article
Chemistry, Multidisciplinary
Rawia Msalmi, Slim Elleuch, Besma Hamdi, Wesam Abd El-Fattah, Naoufel Ben Hamadi, Houcine Naili
Summary: In this work, we report two zero-dimensional Cd-based hybrid compounds with wide-gap semiconductor properties suitable for optoelectronic applications. These materials show wavelength dependent white-light emission behavior, with CdACP exhibiting both fluorescence and room temperature phosphorescence, and CdODA exhibiting purely fluorescence. The ultra-fast fluorescence in CdODA is attributed to intramolecular proton transfer. The optical and luminescence properties of these materials are influenced by the heavy halide effect.