BibTex format
@article{Maimaris:2022:10.1038/s41467-022-32478-8,
author = {Maimaris, M and Pettipher, AJ and Azzouzi, M and Walke, DJ and Zheng, X and Gorodetsky, A and Dong, Y and Tuladhar, Shakya P and Crespo, H and Nelson, J and Tisch, J and Bakulin, A},
doi = {10.1038/s41467-022-32478-8},
journal = {Nature Communications},
title = {Sub-10-fs observation of bound exciton formation in organic optoelectronic devices},
url = {http://dx.doi.org/10.1038/s41467-022-32478-8},
volume = {13},
year = {2022}
}
RIS format (EndNote, RefMan)
TY - JOUR
AB - Fundamental mechanisms underlying exciton formation in organic semiconductors are complex and elusive as it occurs on ultrashort sub-100-fs timescales. Some fundamental aspects of this process, such as the evolution of exciton binding energy, have not been resolved in time experimentally. Here, we apply a combination of sub-10-fs Pump-Push-Photocurrent, Pump-Push-Photoluminescence, and Pump-Probe spectroscopies to polyfluorene devices to track the ultrafast formation of excitons. While Pump-Probe is sensitive to the total concentration of excited states, Pump-Push-Photocurrent and Pump-Push-Photoluminescence are sensitive to bound states only, providing access to exciton binding dynamics. We find that excitons created by near-absorption-edge photons are intrinsically bound states, or become such within 10 fs after excitation. Meanwhile, excitons with a modest >0.3 eV excess energy can dissociate spontaneously within 50 fs before acquiring bound character. These conclusions are supported by excited-state molecular dynamics simulations and a global kinetic model which quantitatively reproduce experimental data.
AU - Maimaris,M
AU - Pettipher,AJ
AU - Azzouzi,M
AU - Walke,DJ
AU - Zheng,X
AU - Gorodetsky,A
AU - Dong,Y
AU - Tuladhar,Shakya P
AU - Crespo,H
AU - Nelson,J
AU - Tisch,J
AU - Bakulin,A
DO - 10.1038/s41467-022-32478-8
PY - 2022///
SN - 2041-1723
TI - Sub-10-fs observation of bound exciton formation in organic optoelectronic devices
T2 - Nature Communications
UR - http://dx.doi.org/10.1038/s41467-022-32478-8
UR - http://hdl.handle.net/10044/1/98875
VL - 13
ER -