Interchromophore Rotation-Related Ultrafast Charge Separation at Excited States in Head-to-Tail Linked Perylene Diimide Dyads

2019 ◽  
Vol 123 (38) ◽  
pp. 23306-23311 ◽  
Author(s):  
Shaomao Fang ◽  
Jiadong Zhou ◽  
Xuehong Zhou ◽  
Cong Wang ◽  
Nianqiang Jiang ◽  
...  
Keyword(s):  
Excited States ◽  
Charge Separation ◽  
Perylene Diimide

Extent of charge separation in suddenly polarized twisted excited states of linear polyenes

1977 ◽  
Vol 99 (11) ◽  
pp. 3587-3596 ◽  
Author(s):  
M. C. Bruni ◽  
J. P. Daudey ◽  
J. Langlet ◽  
J. P. Malrieu ◽  
F. Momicchioli
Keyword(s):  
Excited States ◽  
Charge Separation ◽  
Linear Polyenes

Solvent Induced Charge Separation in the Excited States of Symmetrical Ethylene:  A Direct Reaction Field Study

2001 ◽  
Vol 105 (14) ◽  
pp. 3583-3590 ◽  
Author(s):  
Robert W. J. Zijlstra ◽  
Ferdinand C. Grozema ◽  
Marcel Swart ◽  
Ben L. Feringa ◽  
Piet Th. van Duijnen
Keyword(s):  
Field Study ◽  
Excited States ◽  
Charge Separation ◽  
Direct Reaction ◽  
Reaction Field ◽  
Induced Charge

scholarly journals Spectroscopic investigation of excitonic and charge photogeneration processes in organic photovoltaic cells

2021 ◽  
Author(s):  
◽  
Joseph Gallaher
Keyword(s):  
Excited States ◽  
Charge Separation ◽  
Transient Absorption ◽  
Mirror Image ◽  
Triplet Exciton ◽  
Organic Photovoltaic ◽  
Charge Generation ◽  
Time Resolved ◽  
Blend Morphology ◽  
Time Resolved Photoluminescence

<p>Organic photovoltaic (OPV) cells show significant promise as a renewable energy resource capable of meeting the world’s large and growing energy needs. Increasing device efficiency is central to achieving an economically viable option for widespread applications. To this end, a better understanding of the structure and dynamics of the electronic excited states is needed. In particular, the mechanism by which excitons (electron-hole pairs) escape their Coulombic attraction and generate photocurrent is yet to be established. In this thesis ultrafast laser spectroscopy, in particular transient absorption and time-resolved photoluminescence, are used to study: exciton relaxation, morphological effects on charge separation, and the pathway leading to triplet exciton states.  In Chapter 3, a series of oligothiophenes are synthesised with well-defined conjugation lengths to act as molecular models of polymer backbone sub-units, and thereby probe exciton relaxation processes. Time-resolved photoluminescence (TRPL) and transient absorption (TA) spectroscopy measurements presented in Chapter 4 reveal emission signatures evolve from a mirror image of absorption - which lacks vibronic structure - towards a spectrally narrower and vibronically structured species on the hundreds of femtosecond to early picosecond timescale. Analysis of this spectral evolution shows that a broad distribution of torsional conformers is driven to rapidly planarize in the excited state, including in solid films. This provides evidence that both torsional relaxation and energy migration could contribute to the non-mirror image absorption-emission spectra observed in polymer thin films.  Recently, long lived TA signatures have been attributed to triplet excited states with the suggested formation pathway being similar to organic light emitting diodes, whereby non-geminate (bimolecular) charge recombination leads to the formation of both singlet and triplet states. Isolated oligothiophenes in solution provide an ideal model system to investigate the role of structural relaxation on triplet exciton formation. Through analysis of TA spectral dynamics in Chapter 5, singlet and triplet exciton populations were tracked. Restriction of the torsional relaxation increased triplet yield suggesting vibrational hot states could drive triplet formation. This model could aid in understanding triplet exciton formation in polymer-based solar cells via spin-mixing instead of non-geminate recombination.  In a series of polymer:fullerene blends, the link between the nature of polymerfullerene intermixing and charge generation pathways was investigated. It is shown in Chapter 6 that free charge generation is most efficient in a 3-phase morphology that features intimately mixed polymer:fullerene regions amongst neat polymer and fullerene phases. Distinct spectroscopic signatures made it possible to determine whether holes occupy disordered or crystalline polymer chains. TA spectral dynamics reveal the migration of holes from intermixed to pure olymer regions in 3-phase morphology blends, which contrasted with observations in 2-phase blends. The energy gradient between the intermixed and phase-pure regions may be sufficient to drive efficient separation of charge pairs initially generated in intermixed regions, with free charges subsequently percolating through these phase-pure domains.  The photophysics of a high performance polymer:polymer blend is studied in Chapter 7 in an effort to elucidate how these blends can rival their polymer:fullerene counterparts. Optical spectroscopy reveals incomplete exciton dissociation and rapid geminate recombination in the blends. This is shown to result from a largely phase-separated morphology with domains greater than the exciton diffusion length. Significant loss of charge carriers on early timescales highlights increasing polymer: polymer solar cell efficiency requires optimizing blend morphology to realise facile charge separation.  Taken together, this thesis presents a valuable spectroscopic insight into the pathway of efficient charge separation and the importance of both blend morphology and polymer structure.</p>

Excited-State Symmetry-Breaking Charge Separation Dynamics in Multibranched Perylene Diimide Molecules

2020 ◽  
Vol 11 (24) ◽  
pp. 10329-10339
Author(s):  
Jie Kong ◽  
Wei Zhang ◽  
Gang Li ◽  
Dayujia Huo ◽  
Yuanyuan Guo ◽  
...  
Keyword(s):  
Excited State ◽  
Symmetry Breaking ◽  
Charge Separation ◽  
Perylene Diimide

scholarly journals Occurrence of excited state charge separation in a N-doped graphene–perylenediimide hybrid formed via ‘click’ chemistry

2019 ◽  
Vol 1 (10) ◽  
pp. 4009-4015 ◽  
Author(s):  
Habtom B. Gobeze ◽  
Luis M. Arellano ◽  
Ana María Gutiérrez-Vílchez ◽  
María J. Gómez-Escalonilla ◽  
Ángela Sastre-Santos ◽  
...  
Keyword(s):  
Excited State ◽  
Click Chemistry ◽  
Charge Separation ◽  
Perylene Diimide ◽  
Doped Graphene ◽  
Donor Acceptor ◽  
State Charge

A donor–acceptor hybrid was devised and synthesized using N-doped graphene and perylene diimide via click chemistry, and the occurrence of excited state charge separation is demonstrated.

A Comparison of Charge Separation Dynamics in Organic Blend Films Employing Fullerene and Perylene Diimide Electron Acceptors

2014 ◽  
Vol 6 (1) ◽  
pp. 201-205 ◽  
Author(s):  
Safa Shoaee ◽  
Florent Deledalle ◽  
Pabitra Shakya Tuladhar ◽  
Ravichandran Shivanna ◽  
Sridhar Rajaram ◽  
...  
Keyword(s):  
Charge Separation ◽  
Electron Acceptors ◽  
Perylene Diimide ◽  
Blend Films

scholarly journals Fluorescence quantum yield rationalized by the magnitude of the charge transfer in π-conjugated terpyridine derivatives

2016 ◽  
Vol 18 (42) ◽  
pp. 29387-29394 ◽  
Author(s):  
Marie Humbert-Droz ◽  
Claude Piguet ◽  
Tomasz A. Wesolowski
Keyword(s):  
Dipole Moment ◽  
Charge Transfer ◽  
Quantum Yield ◽  
Excited States ◽  
Charge Separation ◽  
Fluorescence Quantum Yield ◽  
Molecular Design ◽  
Electron Hole ◽  
Two Measures

Two measures of charge separation in ground and excited states (length of the change in dipole moment and the electron–hole distance) provide a remarkable tool for the molecular design of a fluorescent polyaromatic antenna.

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