Nonlinear photophysics and charge generation of donor-acceptor two-photon absorbing dyes

Author(s):  
Sean M. Kirkpatrick ◽  
Elaine K. Peterman ◽  
Gregg T. Anderson ◽  
Jeffrey E. Franklin ◽  
Jeffery W. Baur
Author(s):  
Shahidul Alam ◽  
Vojtech Nádaždy ◽  
Tomáš Váry ◽  
Christian Friebe ◽  
Rico Meitzner ◽  
...  

Energy level alignments at the organic donor–acceptor interface cannot be predicted from cyclic voltammetry. Onsets for joint density of states and charge generation, reveal cases of energy uphill and – newly observed – downhill charge generation.


2019 ◽  
Author(s):  
Pralok K. Samanta ◽  
Md Mehboob Alam ◽  
Ramprasad Misra ◽  
Swapan K. Pati

Solvents play an important role in shaping the intramolecular charge transfer (ICT) properties of π-conjugated molecules, which in turn can affect their one-photon absorption (OPA) and two-photon absorption (TPA) as well as the static (hyper)polarizabilities. Here, we study the effect of solvent and donor-acceptor arrangement on linear and nonlinear optical (NLO) response properties of two novel ICT-based fluorescent sensors, one consisting of hemicyanine and dimethylaniline as electron withdrawing and donating groups (molecule 1), respectively and its boron-dipyrromethene (BODIPY, molecule 2)-fused counterpart (molecule 3). Density functional theoretical (DFT) calculations using long-range corrected CAM-B3LYP and M06-2X functionals, suitable for studying properties of ICT molecules, are employed to calculate the desired properties. The dipole moment (µ) as well as the total first hyperpolarizability (β<sub>total</sub>) of the studied molecules in the gas phase is dominantly dictated by the component in the direction of charge transfer. The ratios of vector component of first hyperpolarizability (β<sub>vec</sub>) to β<sub>total</sub> also reveal unidirectional charge transfer process. The properties of the medium significantly affect the OPA, hyperpolarizability and TPA properties of the studied molecules. Time dependent DFT (TDDFT) calculations suggest interchanging between two lowest excited states of molecule 3 from the gas phase to salvation. The direction of charge polarization and dominant transitions among molecular orbitals involved in the OPA and TPA processes are studied. The results presented are expected to be useful in tuning the NLO response of many ICT-based chromophores, especially those with BODIPY acceptors.<br>


2019 ◽  
Vol 4 (2) ◽  
pp. 449-449
Author(s):  
Brigitte Holzer ◽  
Markus Lunzer ◽  
Arnulf Rosspeintner ◽  
Giuseppe Licari ◽  
Maximilian Tromayer ◽  
...  

Correction for ‘Towards efficient initiators for two-photon induced polymerization: fine tuning of the donor/acceptor properties’ by Brigitte Holzer et al., Mol. Syst. Des. Eng., 2019, DOI: 10.1039/c8me00101d.


2020 ◽  
Vol 124 (45) ◽  
pp. 24631-24643
Author(s):  
Yogajivan Rout ◽  
Alessio Cesaretti ◽  
Elena Ferraguzzi ◽  
Benedetta Carlotti ◽  
Rajneesh Misra

Materials ◽  
2020 ◽  
Vol 13 (7) ◽  
pp. 1727 ◽  
Author(s):  
Ji-Hyun Lee ◽  
Armand Perrot ◽  
Masahiro Hiramoto ◽  
Seiichiro Izawa

Clarifying critical differences in free charge generation and recombination processes between inorganic and organic semiconductors is important for developing efficient organic photoconversion devices such as solar cells (SCs) and photodetector. In this study, we analyzed the dependence of doping concentration on the photoconversion process at the organic pn-homojunction interface in a single organic semiconductor using the temperature dependence of J–V characteristics and energy structure measurements. Even though the organic pn-homojunction SC devices were fabricated using a single host material and the doping technique resembling an inorganic pn-homojunction, the charge generation and recombination mechanisms are similar to that of conventional donor/acceptor (D/A) type organic SCs; that is, the charge separation happens from localized exciton and charge transfer (CT) state being separated by the energy offset between adjacent molecules, and the recombination happens from localized charge carrier at two adjacent molecules. The determining factor for photoconversion processes is the localized nature of charges in organic semiconductors. The results demonstrated that controlling the delocalization of the charges is important to realize efficient organic photoconversion devices.


2015 ◽  
Vol 3 (4) ◽  
pp. 742-749 ◽  
Author(s):  
Anna Purc ◽  
Krzysztof Sobczyk ◽  
Yusuke Sakagami ◽  
Akihiro Ando ◽  
Kenji Kamada ◽  
...  

Decorating diketopyrrolopyrroles with strongly electron-rich heterocycles led to donor–acceptor–donor architectures possessing two-photon brightness 850–1900 GM.


2020 ◽  
Vol 11 (1) ◽  
Author(s):  
Ture F. Hinrichsen ◽  
Christopher C. S. Chan ◽  
Chao Ma ◽  
David Paleček ◽  
Alexander Gillett ◽  
...  

Abstract Organic solar cells based on non-fullerene acceptors can show high charge generation yields despite near-zero donor–acceptor energy offsets to drive charge separation and overcome the mutual Coulomb attraction between electron and hole. Here, we use time-resolved optical spectroscopy to show that free charges in these systems are generated by thermally activated dissociation of interfacial charge-transfer states that occurs over hundreds of picoseconds at room temperature, three orders of magnitude slower than comparable fullerene-based systems. Upon free electron–hole encounters at later times, both charge-transfer states and emissive excitons are regenerated, thus setting up an equilibrium between excitons, charge-transfer states and free charges. Our results suggest that the formation of long-lived and disorder-free charge-transfer states in these systems enables them to operate closely to quasi-thermodynamic conditions with no requirement for energy offsets to drive interfacial charge separation and achieve suppressed non-radiative recombination.


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