Shaped and Feedback-Controlled Excitation of Single Molecules in the Weak-Field Limit

Weigel, Alexander; Sebesta, Aleksandar; Kukura, Philipp

doi:10.1021/acs.jpclett.5b01748

Cited by 34 publications

(37 citation statements)

References 42 publications

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“…This unexpectedly long survival time is rather surprising given that coherences in organic molecules usually persist only for about 50 fs at room temperature. [106,140] To account for these long coherence times in light-harvesting complexes several mechanism were proposed based mainly on results from two-dimensional ensemble spectroscopy. [141][142][143][144][145][146] Initially, this effect was attributed to longlived spatially correlated structural fluctuations of the protein matrix surrounding the involved dyes, which result in longlived site-energy cross-correlations; [143][144][145][146] however, subsequent work provided no evidence for the presence of such correlations.…”

Section: Purple Bacteriamentioning

confidence: 99%

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Brixner

Hildner

Köhler

et al. 2017

Advanced Energy Materials

302

301

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The transport of excitation energy in molecular aggregates is of crucial importance for the function of organic optoelectronic devices and next‐generation solar cells. First, this review summarizes the theoretical background of the nature of the electronically excited states of molecular aggregates. For these systems, the electronic interaction between the monomers leads to the formation of exciton states. This goes along with a shift of the excitation energies and a redistribution of the oscillator strength with respect to the monomers. Next, a brief overview is provided over experimental techniques that allow to study the properties of excitons in molecular aggregates. This includes single‐molecule spectroscopy, coherent two‐dimensional (2D) spectroscopy, and single‐molecule coherent spectroscopy. Finally, examples of molecular aggregates spanning the range from natural systems that act in photosynthesis as light‐harvesting antennas to artificial aggregates built from synthetic chromophores are illustrated.

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Section: Purple Bacteriamentioning

confidence: 99%

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Brixner

Hildner

Köhler

et al. 2017

Advanced Energy Materials

302

301

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“…To investigate as well as to manipulate ultrafast dynamical processes in nanoscale objects, e.g. single molecules or (in)organic nanostructures, coherent control methods provide capabilities beyond conventional spectroscopic methods [1][2][3][4][5][6][7][8][9]. Coherent control refers to the active steering of quantum mechanical processes towards a final desired state.…”

Section: Introductionmentioning

confidence: 99%

“…This approach involves either the suppression or enhancement of transition probabilities within the system investigated by quantum mechanical interference. Hence, quantum processes that can be addressed with coherent control schemes take place on time scales shorter than the effective dephasing time T 2 [7,8,10]. Since in condensed phase at room temperature these time scales are often of the order of some tens of femtoseconds, ultrashort pulsed excitation schemes are required.…”

Section: Introductionmentioning

confidence: 99%

Two-photon induced ultrafast coherence decay of highly excited states in single molecules

et al. 2019

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Coherence is a key aspect of a large variety of processes, ranging from the coherent delocalisation of excitation energy, which is important for energy transfer in supramolecular nanostructures, to coherence between electronic states of a single quantum system, which is essential for quantum optical applications. Coherent control schemes exploit this quantum mechanical property by actively manipulating the outcome of dynamical processes. Moreover, this technique allows measuring dynamical processes under the influence of dephasing. However, going beyond the ensemble averaged situation, i.e. working on the level of single quantum systems, is highly challenging for quantum systems embedded in a solid matrix at elevated temperature. Since interactions between the quantum system and its specific local environment are a priori unknown, this requires a reliable approach to retrieve the relevant parameters governing the ultrafast coherent dynamics. Here, we present measurements of the ultrafast coherence decay of two-photon accessible excited states in single organic molecules embedded in a disordered environment at room temperature. We combine this experimental approach with a quantum dynamics identification procedure, which yields a minimum three-level model to describe the obtained data with very good agreement. In particular, we are able to retrieve the ultrafast (coherent) excited state dynamics in single molecules and demonstrate its sensitivity to the local nanoenvironment from molecule to molecule. This work provides a robust approach to measure and analyse ultrafast quantum dynamics in complex nanosystems.

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“…As a result, different ensembles can be represented by the sameρ, complicating their microscopic interpretation. The importance of this physical insight has been exemplified in the study of light-induced biomolecular dynamics [15][16][17][18][19][20], environment-conditioned qubit dynamics [21], and emerging ultrafast single-molecule spectroscopies [22][23][24][25][26][27].…”

mentioning

confidence: 99%

State space distribution and dynamical flow for closed and open quantum systems

Dodin

Willard

2019

The Journal of Chemical Physics

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We present a general formalism for studying the effects of dynamical heterogeneity in open quantum systems. We develop this formalism in the state space of density operators, on which ensembles of quantum states can be conveniently represented by probability distributions. We describe how this representation reduces ambiguity in the definition of quantum ensembles by providing the ability to explicitly separate classical and quantum sources of probabilistic uncertainty. We then derive explicit equations of motion for state space distributions of both open and closed quantum systems and demonstrate that resulting dynamics take a fluid mechanical form analogous to a classical probability fluid on Hamiltonian phase space, thus enabling a straightforward quantum generalization of Liouville's theorem. We illustrate the utility of our formalism by analyzing the dynamics of an open two-level system using the state-space formalism that are shown to be consistent with the derived analytical results.

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Shaped and Feedback-Controlled Excitation of Single Molecules in the Weak-Field Limit

Cited by 34 publications

References 42 publications

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Exciton Transport in Molecular Aggregates – From Natural Antennas to Synthetic Chromophore Systems

Two-photon induced ultrafast coherence decay of highly excited states in single molecules

State space distribution and dynamical flow for closed and open quantum systems

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