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Cooperative Robustness to Static Disorder: Superradiance and localization in a nanoscale ring to model natural light-harvesting systems  [PDF]
G. L. Celardo,G. G. Giusteri,F. Borgonovi
Physics , 2014, DOI: 10.1103/PhysRevB.90.075113
Abstract: We analyze a 1-d ring structure composed of many two-level systems, in the limit where only one excitation is present. The two-level systems are coupled to a common environment, where the excitation can be lost, which induces super and subradiant behavior, an example of cooperative quantum coherent effect. We consider time-independent random fluctuations of the excitation energies. This static disorder, also called inhomogeneous broadening in literature, induces Anderson localization and is able to quench Superradiance. We identify two different regimes: $i)$ weak opening, in which Superradiance is quenched at the same critical disorder at which the states of the closed system localize; $ii)$ strong opening, with a critical disorder strength proportional to both the system size and the degree of opening, displaying robustness of cooperativity to disorder. Relevance to photosynthetic complexes is discussed.
Interplay between Dephasing and Geometry and Directed Heat Flow in Exciton Transfer Complexes  [PDF]
Yonatan Dubi
Physics , 2015,
Abstract: The striking efficiency of energy transfer in natural photosynthetic systems and the recent evidence of long-lived quantum coherence in biological light harvesting complexes has triggered much excitement, due to the evocative possibility that these systems - essential to practically all life on earth -- use quantum mechanical effects to achieve optimal functionality. A large body of theoretical work has addressed the role of local environments in determining the transport properties of excitons in photosynthetic networks and the survival of quantum coherence in a classical environment. Nonetheless, understanding the connection between quantum coherence, exciton network geometry and energy transfer efficiency remains a challenge. Here we address this connection from the perspective of heat transfer within the exciton network. Using a non-equilibrium open quantum system approach and focusing on the Fenna-Matthews-Olson complex, we demonstrate that finite local dephasing can be beneficial to the overall power output. The mechanism for this enhancement of power output is identified as a gentle balance between quantum and classical contributions to the local heat flow, such that the total heat flow is directed along the shortest paths and dissipation is minimized. Strongly related to the spatial network structure of the exciton transfer complex, this mechanism elucidates how energy flows in photosyntetic excitonic complexes.
Superradiance Transition in Photosynthetic Light-Harvesting Complexes  [PDF]
G. L. Celardo,F. Borgonovi,M. Merkli,V. I. Tsifrinovich,G. P. Berman
Quantitative Biology , 2011, DOI: 10.1021/jp302627w
Abstract: We investigate the role of long-lasting quantum coherence in the efficiency of energy transport at room temperature in Fenna-Matthews-Olson photosynthetic complexes. The excitation energy transfer due to the coupling of the light harvesting complex to the reaction center ("sink") is analyzed using an effective non-Hermitian Hamiltonian. We show that, as the coupling to the reaction center is varied, maximal efficiency in energy transport is achieved in the vicinity of the superradiance transition, characterized by a segregation of the imaginary parts of the eigenvalues of the effective non-Hermitian Hamiltonian. Our results demonstrate that the presence of the sink (which provides a quasi--continuum in the energy spectrum) is the dominant effect in the energy transfer which takes place even in absence of a thermal bath. This approach allows one to study the effects of finite temperature and the effects of any coupling scheme to the reaction center. Moreover, taking into account a realistic electric dipole interaction, we show that the optimal distance from the reaction center to the Fenna-Matthews-Olson system occurs at the superradiance transition, and we show that this is consistent with available experimental data.
Polarized superradiance from delocalized exciton transitions in tetracene single crystals  [PDF]
Andrea Camposeo,Marco Polo,Silvia Tavazzi,Leonardo Silvestri,Peter Spearman,Roberto Cingolani,Dario Pisignano
Physics , 2013, DOI: 10.1103/PhysRevB.81.033306
Abstract: Polarized superradiant emission and exciton delocalization in tetracene single crystals are reported. Polarization-, time-, and temperature-resolved spectroscopy evidence the complete polarization of the zero-phonon line of the intrinsic tetracene emission from both the lower (F state) and the upper (thermally activated) Davydov excitons. The superradiance of the F emission is substantiated by a nearly linear decrease of the radiative lifetime with temperature, being fifteen times shorter at 30 K compared to the isolated molecule, with an exciton delocalization of about 40 molecules.
Nonlinear optical response and exciton dephasing in quantum dots  [PDF]
E. A. Muljarov,R. Zimmermann
Statistics , 2006, DOI: 10.1002/pssb.200668036
Abstract: The full time-dependent four-wave mixing polarization in quantum dots is microscopically calculated, taking into account acoustic phonon-assisted transitions between different exciton states of the dot. It is shown that quite different dephasing times of higher exciton states in pancake anisotropic InGaAs quantum dots are responsible for the experimentally observed [1] double-exponential decay in the photon echo signal.
Nonmonotonic energy harvesting efficiency in biased exciton chains  [PDF]
S. M. Vlaming,V. A. Malyshev,J. Knoester
Physics , 2007, DOI: 10.1063/1.2784556
Abstract: We theoretically study the efficiency of energy harvesting in linear exciton chains with an energy bias, where the initial excitation is taking place at the high-energy end of the chain and the energy is harvested (trapped) at the other end. The efficiency is characterized by means of the average time for the exciton to be trapped after the initial excitation. The exciton transport is treated as the intraband energy relaxation over the states obtained by numerically diagonalizing the Frenkel Hamiltonian that corresponds to the biased chain. The relevant intraband scattering rates are obtained from a linear exciton-phonon interaction. Numerical solution of the Pauli master equation that describes the relaxation and trapping processes, reveals a complicated interplay of factors that determine the overall harvesting efficiency. Specifically, if the trapping step is slower than or comparable to the intraband relaxation, this efficiency shows a nonmonotonic dependence on the bias: it first increases when introducing a bias, reaches a maximum at an optimal bias value, and then decreases again because of dynamic (Bloch) localization of the exciton states. Effects of on-site (diagonal) disorder, leading to Anderson localization, are addressed as well.
Phonon-induced Exciton Dephasing in Quantum Dot Molecules  [PDF]
E. A. Muljarov,T. Takagahara,R. Zimmermann
Physics , 2005, DOI: 10.1103/PhysRevLett.95.177405
Abstract: A new microscopic approach to the optical transitions in quantum dots and quantum dot molecules, which accounts for both diagonal and non-diagonal exciton-phonon interaction, is developed. The cumulant expansion of the linear polarization is generalized to a multilevel system and is applied to calculation of the full time dependence of the polarization and the absorption spectrum. In particular, the broadening of zero-phonon lines is evaluated directly. It is found that in some range of the dot distance real phonon-assisted transitions between exciton states dominate the dephasing, while virtual transitions are of minor importance. The influence of Coulomb interaction, tunneling, and structural asymmetry on the exciton dephasing in quantum dot molecules is analyzed.
Suppression of exciton dephasing in quantum dots through ultrafast multipulse control  [PDF]
Thomas E. Hodgson,Lorenza Viola,Irene D'Amico
Physics , 2008,
Abstract: We investigate the usefulness and viability of the scheme developed by Viola and Lloyd [Phys. Rev. A 58, 2733 (1998)] to control dephasing in the context of exciton-based quantum computation with self-assembled quantum dots. We demonstrate that optical coherence of a confined exciton qubit exposed to phonon-induced dephasing can be substantially enhanced through the application of a simple periodic sequence of control pulses. The shape of the quantum dot has a significant effect on the dephasing properties. Remarkably, we find that quantum dots with parameters optimized for implementing quantum computation are among the most susceptible to dephasing, yet periodic decoupling is most efficient for exactly that type of dot. We also show that the presence of an electric field, which is a necessary ingredient for many exciton-based quantum computing schemes, may further increase the control efficiency. Our results suggest that dynamical decoupling may be a method of choice for robust storage of exciton qubits during idle stages of quantum algorithms.
Exciton dephasing in quantum dots: Coupling to LO phonons via excited states  [PDF]
E. A. Muljarov,R. Zimmermann
Statistics , 2007, DOI: 10.1002/pssb.200777613
Abstract: We have found a novel mechanism of spectral broadening and dephasing in quantum dots (QDs) due to the coupling to longitudinal-optical (LO) phonons. In theory, this mechanism comes into play only if the complete manifold of exciton levels (including those in the wetting-layer continuum) is taken into account. We demonstrate this nontrivial dephasing in different types of QDs, using the exactly solvable quadratic coupling model, here generalized to an arbitrary number of excitonic states.
Spin--flip Limited Exciton Dephasing in CdSe/ZnS Colloidal Quantum Dots  [PDF]
Francesco Masia,Nicolò Accanto,Wolfgang Langbein,Paola Borri
Physics , 2011, DOI: 10.1103/PhysRevLett.108.087401
Abstract: The dephasing time of the lowest bright exciton in CdSe/ZnS wurtzite quantum dots is measured from 5 K to 170 K and compared with density dynamics within the exciton fine structure using a sensitive three-beam four-wave-mixing technique unaffected by spectral diffusion. Pure dephasing via acoustic phonons dominates the initial dynamics, followed by an exponential zero-phonon line dephasing of 109 ps at 5 K, much faster than the ~10 ns exciton radiative lifetime. The zero-phonon line dephasing is explained by phonon-assisted spin-flip from the lowest bright state to dark exciton states. This is confirmed by the temperature dependence of the exciton lifetime and by direct measurements of the bright-dark exciton relaxation. Our results give an unambiguous evidence of the physical origin of the exciton dephasing in these nanocrystals.
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