Mapping Excited-State Dynamics by Coherent Control of a Dendrimer's Photoemission Efficiency
Adaptive laser pulse shaping has enabled impressive control over photophysical processes in complex molecules. However, the optimal pulse shape that emerges rarely offers straightforward insight into the excited-state properties being manipulated. We have shown that the emission quantum yield of a d...
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Published in | Science (American Association for the Advancement of Science) Vol. 326; no. 5950; pp. 263 - 267 |
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Main Authors | , , , |
Format | Journal Article |
Language | English |
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Washington, DC
American Association for the Advancement of Science
09.10.2009
The American Association for the Advancement of Science |
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Abstract | Adaptive laser pulse shaping has enabled impressive control over photophysical processes in complex molecules. However, the optimal pulse shape that emerges rarely offers straightforward insight into the excited-state properties being manipulated. We have shown that the emission quantum yield of a donor-acceptor macromolecule (a phenylene ethynylene dendrimer tethered to perylene) can be enhanced by 15% through iterative phase modulation of the excitation pulse. Furthermore, by analyzing the pulse optimization process and optimal pulse features, we successfully isolated the dominant elements underlying the control mechanism. We demonstrated that a step function in the spectral phase directs the postexcitation dynamics of the donor moiety, thus characterizing the coherent nature of the donor excited state. An accompanying pump-probe experiment implicates a 2+1 photon control pathway, in which the optimal pulse promotes a delayed excitation to a second excited state through favorable quantum interference. |
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AbstractList | Adaptive laser pulse shaping has enabled impressive control over photophysical processes in complex molecules. However, the optimal pulse shape that emerges rarely offers straightforward insight into the excited-state properties being manipulated. We have shown that the emission quantum yield of a donor-acceptor macromolecule (a phenylene ethynylene dendrimer tethered to perylene) can be enhanced by 15% through iterative phase modulation of the excitation pulse. Furthermore, by analyzing the pulse optimization process and optimal pulse features, we successfully isolated the dominant elements underlying the control mechanism. We demonstrated that a step function in the spectral phase directs the postexcitation dynamics of the donor moiety, thus characterizing the coherent nature of the donor excited state. An accompanying pump-probe experiment implicates a 2+1 photon control pathway, in which the optimal pulse promotes a delayed excitation to a second excited state through favorable quantum interference. Adaptive laser pulse shaping has enabled impressive control over photophysical processes in complex molecules. However, the optimal pulse shape that emerges rarely offers straightforward insight into the excited-state properties being manipulated. We have shown that the emission quantum yield of a donor-acceptor macromolecule (a phenylene ethynylene dendrimer tethered to perylene) can be enhanced by 15% through iterative phase modulation of the excitation pulse. Furthermore, by analyzing the pulse optimization process and optimal pulse features, we successfully isolated the dominant elements underlying the control mechanism. We demonstrated that a step function in the spectral phase directs the postexcitation dynamics of the donor moiety, thus characterizing the coherent nature of the donor excited state. An accompanying pump-probe experiment implicates a 2+1 photon control pathway, in which the optimal pulse promotes a delayed excitation to a second excited state through favorable quantum interference. [PUBLICATION ABSTRACT] Phasing-In Emission In keeping with quantum mechanics, the dynamics that ensue when molecules absorb light depend not only on the light's frequency but also its phase, which can manipulate excited state trajectories through interference. Recently, an impressive degree of control has been achieved over complex light absorbers, including proteins, by iteratively adapting the phase of a laser excitation pulse. However, the optimal pulses used are often too complicated to reveal straightforward insights into the systems being manipulated. Kuroda et al. (p. 263 ; see the Perspective by Batista ) applied iterative phase manipulation toward optimizing the photoemission efficiency of a macromolecular donor-acceptor system, followed by statistical analysis to isolate a fairly simple phase function underlying much of the control mechanism. Careful follow-up experiments revealed an intuitive picture of the excited state behavior. A simple manipulation of the phase of a laser pulse optimizes photoemission efficiency in a complex molecule. Adaptive laser pulse shaping has enabled impressive control over photophysical processes in complex molecules. However, the optimal pulse shape that emerges rarely offers straightforward insight into the excited-state properties being manipulated. We have shown that the emission quantum yield of a donor-acceptor macromolecule (a phenylene ethynylene dendrimer tethered to perylene) can be enhanced by 15% through iterative phase modulation of the excitation pulse. Furthermore, by analyzing the pulse optimization process and optimal pulse features, we successfully isolated the dominant elements underlying the control mechanism. We demonstrated that a step function in the spectral phase directs the postexcitation dynamics of the donor moiety, thus characterizing the coherent nature of the donor excited state. An accompanying pump-probe experiment implicates a 2+1 photon control pathway, in which the optimal pulse promotes a delayed excitation to a second excited state through favorable quantum interference. |
Author | Kleiman, Valeria D Peng, Zhonghua Kuroda, Daniel G Singh, C.P |
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Keywords | Pulse shaping Photoemission Quantum optics Photoinduced effect Radiation matter interactions Laser beam applications Excited states Optical pulse Quantum interference phenomena Donor acceptor interaction Dendritic structure |
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Snippet | Adaptive laser pulse shaping has enabled impressive control over photophysical processes in complex molecules. However, the optimal pulse shape that emerges... Phasing-In Emission In keeping with quantum mechanics, the dynamics that ensue when molecules absorb light depend not only on the light's frequency but also... |
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SubjectTerms | Chemical engineering Chemistry Dendrimers Electric fields Electric pulses Emissions Energy transfer Exact sciences and technology Fundamental areas of phenomenology (including applications) General and physical chemistry Lasers Macromolecules Mapping Molecules Nonlinear optics Optics Photochemistry Photons Physical chemistry of induced reactions (with radiations, particles and ultrasonics) Physics Q1 Quantum mechanics Quantum theory Step functions Theory of reactions, general kinetics Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry Ultrafast processes; optical pulse generation and pulse compression |
Title | Mapping Excited-State Dynamics by Coherent Control of a Dendrimer's Photoemission Efficiency |
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