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arXiv:0705.3700 · Physical Review Letters

Survival Probabilities in Coherent Exciton Transfer with Trapping

Oliver Mülken, A. Blumen, Thomas Amthor, Christian Giese, M. Reetz‐Lamour, Matthias Weidemüller

Published Aug 27, 2007• 110 citations
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Abstract

In the quest for signatures of coherent transport we consider exciton trapping in the continuous-time quantum walk framework. The survival probability displays different decay domains, related to distinct regions of the spectrum of the Hamiltonian. For linear systems and at intermediate times the decay obeys a power law, in contrast with the corresponding exponential decay found in incoherent continuous-time random walk situations. To differentiate between the coherent and incoherent mechanisms, we present an experimental protocol based on a frozen Rydberg gas structured by optical dipole traps.

DOI
10.1103/physrevlett.99.090601

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In the quest for signatures of coherent transport we consider exciton trapping in the continuous-time quantum walk framework. The survival probability displays different decay domains, related to distinct regions of the spectrum of the Hamiltonian. For linear systems and at intermediate times the decay obeys a power law, in contrast with the corresponding exponential decay found in incoherent continuous-time random walk situations. To differentiate between the coherent and incoherent mechanisms, we present an experimental protocol based on a frozen Rydberg gas structured by optical dipole traps.
Recent findings suggest that processes such as the excitonic energy transfer through the photosynthetic antenna display quantal features, aspects known from the dynamics of charge carriers along polymer backbones. Hence, in modeling energy transfer one has to leave the classical, master-equation-type formalism and advance towards an increasingly quantum-mechanical picture, while still retaining a local description of the complex network of molecules involved in the transport, say through a tight-binding approach. Interestingly, the continuous time random walk (CTRW) picture, widely employed in describing transport in random environments, can be mathematically reformulated to yield a quantum-mechanical Hamiltonian of tight-binding type; the procedure uses the mathematical analogies between time-evolution operators in statistical and in quantum mechanics: The result are continuous-time quantum walks (CTQWs). However, beyond these formal analogies, CTRWs and CTQWs display vastly different physical properties. In particular, here we focus on trapping processes on a ring and show, both analytically and numerically, that distinct configurations of traps (ranging from periodical to random) yield strongly different behaviors for the quantal mean survival probability, while classically (under ordered conditions) we always find an exponential decay at long times.
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Recent findings suggest that processes such as the electronic energy transfer through the photosynthetic antenna display quantal features, aspects known from the dynamics of charge carriers along polymer backbones. Hence, in modeling energy transfer one has to leave the classical, masterequation-type formalism and advance towards an increasingly quantum-mechanical picture, while still retaining a local description of the complex network of molecules involved in the transport, say through a tight-binding approach. Interestingly, the continuous time random walk (CTRW) picture, widely employed in describing transport in random environments, can be mathematically reformulated to yield a quantummechanical Hamiltonian of tight-binding type; the procedure uses the mathematical analogies between time-evolution operators in statistical and in quantum mechanics: The result are continuoustime quantum walks (CTQWs). However, beyond these formal analogies, CTRWs and CTQWs display vastly different physical properties. In particular, here we focus on trapping processes on a ring and show, both analytically and numerically, that distinct configurations of traps (ranging from periodical to random) yield strongly different behaviours for the quantal mean survival probability, while classically (under ordered conditions) we always find an exponential decay at long times.
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Coherent transport of excitations along chains of coupled quantum systems represents an interesting problem with a number of applications ranging from quantum optics to solar cell technology. A convenient tool for studying such processes are quantum walks. They allow us to determine all the process features in a quantitative way. We study the survival probability and the transport efficiency on a simple, highly symmetric graph represented by a ring. The propagation of excitation is modeled by a discrete-time (coined) quantum walk. For a two-state quantum walk, where the excitation (walker) has to leave its actual position to the neighboring sites, the survival probability decays exponentially and the transport efficiency is unity. The decay rate of the survival probability can be estimated using the leading eigenvalue of the evolution operator. However, if the excitation is allowed to stay at its present position, i.e. the propagation is modeled by a lazy quantum walk, then part of the wave-packet can be trapped in the vicinity of the origin and never reaches the sink. In such a case, the survival probability does not vanish and the excitation transport is not efficient. The dependency of the transport efficiency on the initial state is determined. Nevertheless, we show that for some lazy quantum walks dynamical, percolations of the ring eliminate the trapping effect and efficient excitation transport can be achieved.
We study the coherent exciton transport of continuous-time quantum walks (CTQWs) on Erdos-Renyi networks. The Erdos-Renyi network of N nodes is constructed by connecting every pair of nodes with probability ppp. We numerically calculate the ensemble averaged transition probability of quantum transport between two nodes of the networks. For finite networks, we find that the limiting transition probability is reached very quickly. For infinite networks whose spectral density follows the semicircle law, the efficiencies of the classical and quantum-mechanical transport are compared on networks of different average degree. In the long time limiting, we consider the distribution of the ensemble averaged transition probabilities, and show that there is a high probability to find the exciton at the initial node. Such high return probability almost do not alter in a wide range of connection probability p but increases rapidly when the network approaches to be fully connected. For networks whose topology is not extremely connected, the return probability is inversely proportional to the network size N. Furthermore, the transport dynamics are compared with that on a random graph model in which the degree of each node equals to the average degree of the Erdos-Renyi networks.