TY - JOUR
T1 - Spatial Correlations Drive Long-Range Transport and Trapping of Excitons in Single H‑Aggregates
T2 - Experiment and Theory
AU - Carta, Alberto
AU - Wittmann, Bernd
AU - Kreger, Klaus
AU - Schmidt, Hans-Werner
AU - Jansen, Thomas L. C.
AU - Hildner, Richard
PY - 2024/3/14
Y1 - 2024/3/14
N2 - Describinglong-rangeenergytransportis a crucialstep, both towarddeepeningour knowledgeon naturallight-harvestingsystemsand towarddevelopingnovel photoactivematerials.Here, we combineexperimentand theoryto resolveand reproduceenergytransporton pico- to nanosecondtime scalesin singleH-typesupramolecularnanofibersbasedoncarbonyl-bridgedtriarylamines(CBT).Each nanofibershowsenergytransportdynamicsoverlong distancesup to∼1μm, despiteexcitontrappingat specificpositionsalong the nanofibers.Usinga minimalFrenkelexcitonmodelincludingdisorder,we demonstratethat spatialcorrelationsin the normallydistributedsite energiesare crucialto reproducethe experimentaldata. In particular,we can observethe long-rangeand subdiffusivenatureof the excitondynamicsas well as the trappingbehaviorof excitonsin specificlocationsof the nanofiber.Thistrappingbehaviorintroducesa net directionalityor asymmetryin the excitondynamicsasobservedexperimentally.
AB - Describinglong-rangeenergytransportis a crucialstep, both towarddeepeningour knowledgeon naturallight-harvestingsystemsand towarddevelopingnovel photoactivematerials.Here, we combineexperimentand theoryto resolveand reproduceenergytransporton pico- to nanosecondtime scalesin singleH-typesupramolecularnanofibersbasedoncarbonyl-bridgedtriarylamines(CBT).Each nanofibershowsenergytransportdynamicsoverlong distancesup to∼1μm, despiteexcitontrappingat specificpositionsalong the nanofibers.Usinga minimalFrenkelexcitonmodelincludingdisorder,we demonstratethat spatialcorrelationsin the normallydistributedsite energiesare crucialto reproducethe experimentaldata. In particular,we can observethe long-rangeand subdiffusivenatureof the excitondynamicsas well as the trappingbehaviorof excitonsin specificlocationsof the nanofiber.Thistrappingbehaviorintroducesa net directionalityor asymmetryin the excitondynamicsasobservedexperimentally.
KW - SUPRAMOLECULAR ARCHITECTURES
KW - Energy transport
KW - quantum chemical calculations
KW - OPTICAL SPECTROSCOPY
KW - OPTICAL MICROSCOPY
U2 - 10.1021/acs.jpclett.3c03586
DO - 10.1021/acs.jpclett.3c03586
M3 - Article
SN - 1948-7185
VL - 15
SP - 2697
EP - 2707
JO - The Journal of Physical Chemistry Letters
JF - The Journal of Physical Chemistry Letters
ER -