Ultrafast exciton dynamics of <i>J</i>-aggregates in room temperature solution studied by third-order nonlinear optical spectroscopy and numerical simulation based on exciton theory

Ohta, Kaoru; Yang, Mino; Fleming, Graham R.

doi:10.1063/1.1403693

Cited by 81 publications

(95 citation statements)

References 55 publications

(98 reference statements)

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“…In this case, fluorescence emission is observed in resonance to the lowest energy exciton state. The extended exciton states give rise to many peculiar linear and nonlinear optical properties, such as resonant fluorescence [1,2], super radiant emission [7][8][9], high nonlinear susceptibilities [10], efficient exciton-exciton annihilation [11], and energy migration [12][13][14][15]. The latter was already observed by Scheibe et al [16].…”

Section: Introductionmentioning

confidence: 48%

Photo-induced reduction of Noble metal ions to metal nanoparticles on tubular J-aggregates

Kirstein

Berlepsch

Böttcher

2006

International Journal of Photoenergy

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Palladium and silver nanoparticles are formed on the surface of tubular J-aggregates of an amphiphilic tetrachlorobenzimidacarbocyanine dye by reduction of the respective metal cations in aqueous solution. Upon addition of the palladium complex Na 2 PdCl 4 to the aggregate solution, the absorption spectrum shows significant changes which is explained by partial destruction of the aggregates. Cryogenic transmission electron microscopy (cryo-TEM) images show that the tubular J-aggregates are randomly covered by well-separated Pd nanoparticles of approximately 1-3 nm size. Larger particles and higher particle density along the aggregates are obtained when an auxiliary reducing agent is added to the solution. The presence of the metallic particles leads to efficient fluorescence quenching giving clear evidence for super quenching. In similar experiments using AgNO 3 , silver nanoparticles are grown which are larger in size but less dense distributed along the aggregates. At least in the case of the silver particles, the spontaneous formation of metal nanoparticles is assumed to be initiated by a photo-induced electron transfer process (PET).

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Section: Introductionmentioning

confidence: 48%

Photo-induced reduction of Noble metal ions to metal nanoparticles on tubular J-aggregates

Kirstein

Berlepsch

Böttcher

2006

International Journal of Photoenergy

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“…Therefore, the properties of the final thermalized exciton result from the action of both static and dynamic disorder. The combined effects of these parameters on exciton dynamics have been studied so far theoretically [12] and by means of bulk spectroscopy [13]. In bulk experiments, however, the interplay of static and dynamic disorder cannot be disentangled since the average over a wide range of energy differences from molecule to molecule is measured.…”

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confidence: 99%

Effect of Disorder on Ultrafast Exciton Dynamics Probed by Single Molecule Spectroscopy

et al. 2006

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We present a single-molecule study unraveling the effect of static disorder on the vibrational-assisted ultrafast exciton dynamics in multichromophoric systems. For every single complex, we probe the initial exciton relaxation process by an ultrafast pump-probe approach and the coupling to vibrational modes by emission spectra, while fluorescence lifetime analysis measures the amount of static disorder. Exploiting the wide range of disorder found from complex to complex, we demonstrate that static disorder accelerates the dephasing and energy relaxation rate of the exciton. DOI: 10.1103/PhysRevLett.97.216403 PACS numbers: 71.35.Aa, 32.50.+d, 78.47.+p For many decades assemblies of coupled emitters have been studied intensively due to their intriguing properties of spectral narrowing [1] and enhancement of spontaneous emission rate (superradiance) [2]. This behavior stems from coherent excited state energy (exciton) delocalization over the aggregate [3,4]. The exploitation of exciton delocalization for a controlled transfer of energy in photonics and electronics devices as well as in novel schemes for quantum computation has sparked new interest in a wide variety of multichromophoric assemblies, such as photonic polymers [5], light harvesting complexes [6], and quantum dot arrays [7]. In practice, the performance of these systems depends on the extent of coherent exciton delocalization, a property varying in time and space due to static and dynamic disorder [8,9]. Understanding how these two parameters constrain the extent of collective excited states in multichromophoric assemblies is therefore a crucial step in the design of functional excitonically based molecular devices.Static disorder in dye assemblies mainly arises from differences in the energy of the interacting chromophores. The initial exciton created upon absorption is then confined to a region smaller than the actual size of the complex [10]. Coupling of this state to molecular vibrations and bath phonon modes (dynamic disorder) leads to subsequent ultrafast dephasing and energy relaxation through the exciton band. As a consequence, the coherence size of the exciton is further reduced [11]. Therefore, the properties of the final thermalized exciton result from the action of both static and dynamic disorder. The combined effects of these parameters on exciton dynamics have been studied so far theoretically [12] and by means of bulk spectroscopy [13]. In bulk experiments, however, the interplay of static and dynamic disorder cannot be disentangled since the average over a wide range of energy differences from molecule to molecule is measured.In this Letter we investigate the effect of static disorder on exciton dynamics in a multichromophoric system using a unique combination of several room-temperature singlemolecule spectroscopy (SMS) techniques. The coherent delocalization length of the final thermalized exciton is probed using steady-state and fast SMS methods, thus unraveling the extent of static disorder in individual aggregates. The interpla...

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“…[7][8][9] In parallel with these developments, a simpler technique, the two-color photon echo peak shift technique, was developed. [10][11][12][13] This method at first sight seems an almost trivial extension of the photon echo peak shift method (3 PEPS) originally proposed for Markovian systems by Yajima 14 and Ippen and Weiner 15 and developed by ourselves [16][17][18][19] and Wiersma and co-workers 20 for non-Markovian systems. However, this technique, 2C3PEPS, turns out to be a complementary method to 2D photon echo spectroscopy, providing information on the spatial overlap of electronic states, mixing coefficients, and remarkably, pathway-dependent information on the spectral evolution of a dynamical system.…”

Section: Introductionmentioning

confidence: 99%

Two Dimensional Electronic Spectroscopy of Molecular Complexes

Cho¹,

Brixner²,

Stiopkin³

et al. 2006

J Chinese Chemical Soc

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Two dimensional (2D) heterodyne-detected electronic photon echo spectroscopy is introduced and described. We give an intuitive description of the origin and information content of 2D electronic spectra, focusing on molecular complexes. We identify two important quantities-the transition dipole term, and the transition frequency cross correlation function that controls the appearance of 2D electronic spectra.We also show how the transition frequency cross correlation function controls the rate of exciton relaxation. These concepts are illustrated with experimental data on the seven bacteriochlorophyll FMO complex of a green sulfur bacterium, showing how the pathways and mechanisms of energy flow can be elucidated by combining 2D spectra with theoretical modeling.

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Ultrafast exciton dynamics of J-aggregates in room temperature solution studied by third-order nonlinear optical spectroscopy and numerical simulation based on exciton theory

Cited by 81 publications

References 55 publications

Photo-induced reduction of Noble metal ions to metal nanoparticles on tubular J-aggregates

Photo-induced reduction of Noble metal ions to metal nanoparticles on tubular J-aggregates

Effect of Disorder on Ultrafast Exciton Dynamics Probed by Single Molecule Spectroscopy

Two Dimensional Electronic Spectroscopy of Molecular Complexes

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