Ultrafast single-molecule photonics: Excited state dynamics in coherently coupled complexes

Hernando, Jordi; Hoogenboom, Jacob P.; Dijk, Erik van; García-Parajo, María F.; Hulst, Niek F. van

doi:10.1016/j.jlumin.2007.11.027

Cited by 4 publications

(3 citation statements)

References 12 publications

(22 reference statements)

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“…In the case of L3 , among the 37 molecules measured 16 molecules show sequentially blue-shifted fluorescence spectra (Figure a) during photobleaching, indicating that the PDI units are strongly coupled. − These molecules likely follow the photobleaching sequence as described in Figure S3a, Supporting Information, i.e., starting from the terminal PDI unit. In this case, the intermediate dimer also emits red-shifted fluorescence as compared with monomer as a result of exciton delocalization.…”

Section: Resultsmentioning

confidence: 98%

Excitonic Coupling in Linear and Trefoil Trimer Perylenediimide Molecules Probed by Single-Molecule Spectroscopy

et al. 2012

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Perylenediimide (PDI) molecules are promising building blocks for photophysical studies of electronic interactions within multichromophore arrays. Such PDI arrays are important materials for fabrication of molecular nanodevices such as organic light-emitting diodes, organic semiconductors, and biosensors because of their high photostability, chemical and physical inertness, electron affinity, and high tinctorial strength over the entire visible spectrum. In this work, PDIs have been organized into linear (L3) and trefoil (T3) trimer molecules and investigated by single-molecule fluorescence microscopy to probe the relationship between molecular structures and interchromophoric electronic interactions. We found a broad distribution of coupling strengths in both L3 and T3 and hence strong/weak coupling between PDI units by monitoring spectral peak shifts in single-molecule fluorescence spectra upon sequential photobleaching of each constituent chromophore. In addition, we used a wide-field defocused imaging technique to resolve heterogeneities in molecular structures of L3 and T3 embedded in a PMMA polymer matrix. A systematic comparison between the two sets of experimental results allowed us to infer the correlation between intermolecular interactions and molecular structures. Our results show control of the PDI intermolecular interactions using suitable multichromophoric structures.

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Section: Resultsmentioning

confidence: 98%

Excitonic Coupling in Linear and Trefoil Trimer Perylenediimide Molecules Probed by Single-Molecule Spectroscopy

et al. 2012

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“…These coherences were clearly found to influence fluorescence lifetimes as well as the emission spectra . Further interesting photophysical studies of in-line arranged PBI ensembles, in particular with trimer analogues similar to 2-1a , were performed by Matile, Hulst, Hoogenboom, and Garcia-Parajó, − Müllen, De Schryver, and Hofkens, Debije and Schenning, , Herz, and their co-workers. It has been convincingly shown that the degree of PBI dye alignment in a nematic liquid-crystalline host could be appreciably improved by attaching PBI units through rigid N–N linkage as in PBI dimer 2-1a and its trimer analogue .…”

Section: Linear Dendritic and Macrocyclic Covalent Pbi Ensemblesmentioning

confidence: 93%

Perylene Bisimide Dye Assemblies as Archetype Functional Supramolecular Materials

et al. 2015

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CONTENTS 1. Introduction 962 1.1. Prologue 962 1.2. Parent Perylene Bisimide Chromophore 963 1.3. Core-Substituted Perylene Bisimides 964 1.4. Perylene Bisimides in the Solid State 966 1.5. Areas of Application 966 2. Linear, Dendritic, and Macrocyclic Covalent PBI Ensembles 968 2.1. Excitonic Coupling and Deactivation Processes of Photoexcited PBIs 969 2.2. Rigid PBI Dimers 971 2.3. Flexible PBI Ensembles 974 2.4. Cyclic PBI Ensembles 976 3. π-Stacked PBI Assemblies 979 3.1. Self-Assembly of Core-Unsubstituted PBIs in Solution 979 3.2. Organization of Core-Unsubstituted PBIs in the Bulk Solid State 984 3.3. Self-Assembly of Amphiphilic PBIs in Aqueous Media and Solid Bulk State 987 3.4. Self-Assembly of Core-Substituted PBIs 991 3.5. Self-Assembly of Dye Arrays Composed of Multiple PBIs 995 3.6. Self-Assembly of Multichromophoric PBI Conjugates Containing Other Dyes 996 4. Hydrogen-Bond Directed Self-Assembly 1000 4.1. Self-Assembly Directed by Imide−Imide H-Bonding Interactions 1000 4.2. Self-Assembly Directed by Side-Chain Amide−Amide H-Bonding Interactions 1003 4.3. Self-Assembly Directed by Other H-Bonding Interactions 1006 4.4. Coassembly Directed by Imide−Melamine H-Bonding Interactions 1008 4.5. Coassembly Directed by Melamine−Cyanurate/Barbiturate H-Bonding Interactions 1011

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“…The importance of molecular vibrations for energy transfer has been corroborated by recent ultrafast studies of similar PBI systems with orthogonally oriented dipole moments, one of which is parallel to the distance vector R 72. 73 Another notable exception from the Förster treatment are the time‐resolved single‐molecule studies carried out in the group of van Hulst,74, 75 which addressed the effect of static disorder and the role of vibrational modes in coherently coupled PBI complexes. The actual involved degree of coherence cannot be conclusively discussed from our present data.…”

Section: Discussionmentioning

confidence: 96%

Similarities and Differences in the Optical Response of Perylene‐Based Hetero‐Bichromophores and Their Monomeric Units

et al. 2013

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The linear and nonlinear optical response of molecular hetero-dimers and their composing perylene units is explored with fluorometry, steady-state and transient absorption, and coherent two-dimensional electronic spectroscopy. Supported by a Förster theory approach and ab initio calculations, we disclose the photoinduced dynamics comprising excitonic coupling, conformational changes, charge transfer, and relaxation dynamics. The influence of the actual orientation of the two chromophore units on these processes is investigated by employing two bichromophores built of the same monomeric units but linked differently.

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Ultrafast single-molecule photonics: Excited state dynamics in coherently coupled complexes

Cited by 4 publications

References 12 publications

Excitonic Coupling in Linear and Trefoil Trimer Perylenediimide Molecules Probed by Single-Molecule Spectroscopy

Excitonic Coupling in Linear and Trefoil Trimer Perylenediimide Molecules Probed by Single-Molecule Spectroscopy

Perylene Bisimide Dye Assemblies as Archetype Functional Supramolecular Materials

Similarities and Differences in the Optical Response of Perylene‐Based Hetero‐Bichromophores and Their Monomeric Units

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