Mapping of exciton–exciton annihilation in a molecular dimer via fifth-order femtosecond two-dimensional spectroscopy

Suss, J.T.; Wehner, J.; Dostál, Jakub; Brixner, Tobias; Engel, Volker

doi:10.1063/1.5086151

Cited by 24 publications

(12 citation statements)

References 71 publications

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“…This effective repulsion between Frenkel excitons dominates Coulomb interactions between them if the difference in the permanent dipole between the ground and excited states considered is zero. EEA opens a relaxation channel between the | ii 〉 and | i 〉 states 28,31,32,43 . Next to the re-appearance of the otherwise mutually annulled Feynman diagrams, this leads to new diagrams as shown in Fig.…”

Section: Resultsmentioning

confidence: 99%

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

et al. 2019

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Unraveling the nature of energy transport in multi-chromophoric photosynthetic complexes is essential to extract valuable design blueprints for light-harvesting applications. Long-range exciton transport in such systems is facilitated by a combination of delocalized excitation wavefunctions (excitons) and exciton diffusion. The unambiguous identification of the exciton transport is intrinsically challenging due to the system’s sheer complexity. Here we address this challenge by employing a spectroscopic lab-on-a-chip approach: ultrafast coherent two-dimensional spectroscopy and microfluidics working in tandem with theoretical modeling. We show that at low excitation fluences, the outer layer acts as an exciton antenna supplying excitons to the inner tube, while under high excitation fluences the former converts its functionality into an exciton annihilator which depletes the exciton population prior to any exciton transfer. Our findings shed light on the excitonic trajectories across different sub-units of a multi-layered artificial light-harvesting complex and underpin their great potential for directional excitation energy transport.

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Section: Resultsmentioning

confidence: 99%

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

et al. 2019

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“…This technique facilitates a direct observation of exciton-exciton interactions. [48][49][50] In EEI2D, exciton-exciton annihilation is observable in the evolution of the signal amplitude as a function of population time. This technique can therefore be used not only to study EEI, but one can utilize the annihilation as a tool to probe single-exciton propagation dynamics even in the absence of spectral changes during transport.…”

Section: Introductionmentioning

confidence: 99%

From wavelike to sub-diffusive motion: exciton dynamics and interaction in squaraine copolymers of varying length

et al. 2020

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“…We consider the same model system as in Ref. 50, and show that when optical pulses have slightly longer durations than considered in that work, neither the impulsive limit nor the time-ordered diagrams with pulse-shape effects included accurately predict spectra. The calculation with all 240 diagrams requires less than twice the time as using only the 7 time-ordered diagrams despite considering 34 times as many diagrams.…”

Section: Introductionmentioning

confidence: 89%

Automatic Feynman diagram generation for nonlinear optical spectroscopies

Rose,

Krich

2020

Preprint

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Perturbative nonlinear optical spectroscopies are powerful methods to understand the dynamics of excitonic and other condensed phase systems. Feynman diagrams have long provided the essential tool to understand and interpret experimental spectra and to organize the calculation of spectra for model systems. When optical pulses are strictly time ordered, only a small number of diagrams contribute, but in many experiments pulse-overlap effects are important for interpreting results. When pulses overlap, the number of contributing diagrams can increase rapidly, especially with higher order spectroscopies, and human error is especially likely when attempting to write down all of the diagrams. We present an automated Diagram Generator (DG) that generates all of the Feynman diagrams needed to calculate any n th -order spectroscopic signal. We characterize all perturbative nonlinear spectroscopies by their associated phase-discrimination condition as well as the time intervals where pulse amplitudes are nonzero. Although the DG can be used to automate impulsive calculations, its greatest strength lies in automating finite-pulse calculations where pulse overlaps are important. We consider the cases of third-order 2D photon echo spectroscopy and fifth-order exciton-exciton interaction 2D spectroscopy, which are respectively described by 6 or 7 diagrams in the impulsive limit but 16 or 240 diagrams, respectively, when pulses overlap. The DG allows users to automatically include all relevant diagrams at relatively low computational cost, since the extra diagrams are only generated for the inter-pulse delays where they are relevant.

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Mapping of exciton–exciton annihilation in a molecular dimer via fifth-order femtosecond two-dimensional spectroscopy

Cited by 24 publications

References 71 publications

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

Interplay between structural hierarchy and exciton diffusion in artificial light harvesting

From wavelike to sub-diffusive motion: exciton dynamics and interaction in squaraine copolymers of varying length

Automatic Feynman diagram generation for nonlinear optical spectroscopies

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