Efficient energy transport in an organic semiconductor mediated by transient exciton delocalisation

Author(s):  
Alexander Sneyd ◽  
Tomoya Fukui ◽  
David Paleček ◽  
Suryoday Prodhan ◽  
Isabella Wagner ◽  
...  
2021 ◽  
Vol 7 (32) ◽  
pp. eabh4232
Author(s):  
Alexander J. Sneyd ◽  
Tomoya Fukui ◽  
David Paleček ◽  
Suryoday Prodhan ◽  
Isabella Wagner ◽  
...  

Efficient energy transport is desirable in organic semiconductor (OSC) devices. However, photogenerated excitons in OSC films mostly occupy highly localized states, limiting exciton diffusion coefficients to below ~10−2 cm2/s and diffusion lengths below ~50 nm. We use ultrafast optical microscopy and nonadiabatic molecular dynamics simulations to study well-ordered poly(3-hexylthiophene) nanofiber films prepared using living crystallization-driven self-assembly, and reveal a highly efficient energy transport regime: transient exciton delocalization, where energy exchange with vibrational modes allows excitons to temporarily re-access spatially extended states under equilibrium conditions. We show that this enables exciton diffusion constants up to 1.1 ± 0.1 cm2/s and diffusion lengths of 300 ± 50 nm. Our results reveal the dynamic interplay between localized and delocalized exciton configurations at equilibrium conditions, calling for a re-evaluation of exciton dynamics and suggesting design rules to engineer efficient energy transport in OSC device architectures not based on restrictive bulk heterojunctions.


2020 ◽  
Vol 32 (28) ◽  
pp. 2002127
Author(s):  
Shaocong Hou ◽  
Mandeep Khatoniar ◽  
Kan Ding ◽  
Yue Qu ◽  
Alexander Napolov ◽  
...  

2011 ◽  
Author(s):  
Apoorva D. Patel ◽  
Dipankar Home ◽  
Guruprasad Kar ◽  
Archan S. Majumda

2019 ◽  
Vol 10 (45) ◽  
pp. 10503-10509 ◽  
Author(s):  
Shawn Irgen-Gioro ◽  
Karthik Gururangan ◽  
Rafael G. Saer ◽  
Robert E. Blankenship ◽  
Elad Harel

The study of coherence between excitonic states in naturally occurring photosynthetic systems offers tantalizing prospects for uncovering mechanisms of efficient energy transport.


2020 ◽  
Vol 6 (14) ◽  
pp. eaaz4888 ◽  
Author(s):  
Jianshu Cao ◽  
Richard J. Cogdell ◽  
David F. Coker ◽  
Hong-Guang Duan ◽  
Jürgen Hauer ◽  
...  

Photosynthesis is a highly optimized process from which valuable lessons can be learned about the operating principles in nature. Its primary steps involve energy transport operating near theoretical quantum limits in efficiency. Recently, extensive research was motivated by the hypothesis that nature used quantum coherences to direct energy transfer. This body of work, a cornerstone for the field of quantum biology, rests on the interpretation of small-amplitude oscillations in two-dimensional electronic spectra of photosynthetic complexes. This Review discusses recent work reexamining these claims and demonstrates that interexciton coherences are too short lived to have any functional significance in photosynthetic energy transfer. Instead, the observed long-lived coherences originate from impulsively excited vibrations, generally observed in femtosecond spectroscopy. These efforts, collectively, lead to a more detailed understanding of the quantum aspects of dissipation. Nature, rather than trying to avoid dissipation, exploits it via engineering of exciton-bath interaction to create efficient energy flow.


2021 ◽  
Author(s):  
Hülya Ucar ◽  
Hans-Achim Wagenknecht

Two conjugates of tetraphenylethylene with D-2’-deoxyuridine (1D) and L-2’-deoxyuridine (1L) were synthesized to construct new supramolecular DNA-architectures by self-assembly. The non-templated assemblies of 1D and 1L show strong aggregation-induced emission...


2010 ◽  
Vol 83 (1) ◽  
pp. 43-55 ◽  
Author(s):  
An Thien Ngo ◽  
Pierre Karam ◽  
Gonzalo Cosa

Fluorescent conjugated polyelectrolytes (CPEs) have attracted considerable interest over the past decade as novel materials for developing biosensing schemes and sensing devices for biomolecules. This interest stems from the exquisite polymer sensitivity to the presence of fluorescence quenchers, enabling amplified sensing of molecules of interest. Efficient energy transport along the polymer backbone is critical to their sensing capabilities. Considerable research efforts have thus gone into understanding and controlling energy transport along the polymer backbone. In particular, it has been shown that interactions between CPEs with either surfactants or lipid molecules may significantly reduce energy transport along the polymer backbone that in turn may provide for unique biosensing opportunities. In the first half of this review, we give a historical overview on energy transport in conjugated polymers and polyelectrolytes. In the second half, we summarize the most recent work on the interaction of CPEs with surfactants with an emphasis on our own work elucidating electronic energy transport in CPEs encapsulated into lipid vesicles or embedded within the membrane of lipid vesicles.


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