Recently, the quantum nature in the energy transport in solar cells and light-harvesting complexe... more Recently, the quantum nature in the energy transport in solar cells and light-harvesting complexes has attracted much attention as being triggered by the experimental observations. We model the light-harvesting complex (i.e., PEB50 dimer) as a quantum heat engine (QHE) and study the effect of the undamped intramolecule vibrational modes on the coherent energy-transfer process and quantum transport. We find that the exciton−vibration interaction has nontrivial contribution to the promotion of quantum yield as well as transport properties of the QHE at steady state by enhancing the quantum coherence quantified by entanglement entropy. The perfect quantum yield over 90% has been obtained, with the exciton−vibration coupling. We attribute these improvements to the renormalization of the electronic couplings effectively induced by exciton−vibration interaction and the subsequent delocalization of excitons. Finally, we demonstrate that the thermal relaxation and dephasing can help the excitation energy transfer in the PEB50 dimer.
Wedevelop a population and flux landscape theory for general non-equilibrium quantum systems. We ... more Wedevelop a population and flux landscape theory for general non-equilibrium quantum systems. We illustrate our theory by modelling the quantum transport of donor-acceptor energy transfer.We find two driving forces for the non-equilibrium quantum dynamics. The symmetric part of the driving force corresponds to the population landscape contribution which mainly governs the equilibrium part of dynamics while the anti-symmetric part of the driving force generates the non-equilibrium curl quantum flux which leads to the detailed-balance-breaking and time-irreversibility. The multiloop structure of the flux emerges forms the flux-landscape. Westudy the trend of changes in population and flux-landscape with respect to the voltage (temperature difference induced by environments) and electronic coupling. Improving the voltage and electronic coupling in general facilitates the quantum transport by reducing the population landscape barriers between major states and increasing the mean value of the flux. Alimit-cycle mode emerges when the underlying fluxlandscape becomes funnelled with a significant gap between the largest flux loop and the rest of them. On the kinetic level, we find that multiple kinetic paths between quantum states emerge and illustrate the interference effects. The degree of interference is determined by the landscape and flux. Furthermore, we quantify kinetic rate which strongly correlates with the population landscape and flux. For quantum transport, we demonstrate that as the coherence or the quantum entanglement is enhanced, the flux and energy transfer efficiency are increased. Finally it is surprising that the nonequilibriumness quantified by voltage has a non-trivial contribution on strengthening the entanglement, which is attributed to the non-local feature of the quantum curl flux.
We established a theoretical framework in terms of the curl flux, population landscape, and coher... more We established a theoretical framework in terms of the curl flux, population landscape, and coherence for non-equilibrium quantum systems at steady state, through exploring the energy and charge transport in molecular processes. The curl quantum flux plays the key role in determining transport properties and the system reaches equilibrium when flux vanishes. The novel curl quantum flux reflects the degree of non-equilibriumness and the time-irreversibility. We found an analytical expression for the quantum flux and its relationship to the environmental pumping (non-equilibriumness quantified by the voltage away from the equilibrium) and the quantum tunneling. Furthermore, we investigated another quantum signature, the coherence, quantitatively measured by the non-zero off
diagonal element of the density matrix. Populations of states give the probabilities of individual states and therefore quantify the population landscape. Both curl flux and coherence depend on steady state population landscape. Besides the environment-assistance which can give dramatic enhancement of coherence and quantum flux with high voltage at a fixed tunneling strength, the quantum flux is promoted by the coherence in the regime of small tunneling while reduced by the coherence in the regime of large tunneling, due to the non-monotonic relationship between the coherence and tunneling. This is in contrast to the previously found linear relationship. For the systems coupled to bosonic (photonic and phononic) reservoirs the flux is significantly promoted at large voltage while for fermionic (electronic) reservoirs the flux reaches a saturation after a significant enhancement at large voltage due to the Pauli exclusion principle. In view of the system as a quantum heat engine, we studied the non-equilibrium thermodynamics and established the analytical connections of curl quantum flux to the transport quantities such as energy (charge) transfer efficiency, chemical reaction
efficiency, energy dissipation, heat and electric currents observed in the experiments. We observed a perfect transfer efficiency in chemical reactions at high voltage (chemical potential difference). Our theoretical predicted behavior of the electric current with respect to the voltage is in good agreements with the recent experiments on electron transfer in single molecules.
In this article, we consider the monopole excitations of a harmonically trapped Bose gas in the v... more In this article, we consider the monopole excitations of a harmonically trapped Bose gas in the vicinity of the Tonks-Girardeau limit. Using Girardeau’s Fermi-Bose duality and subsequently an effective fermion-fermion odd-wave interaction, we obtain the dominant correction to the scale-invariance-protected value of the excitation frequency, for microscopically small excitation amplitudes. We produce a series of diffusion Monte Carlo results that confirm our analytic prediction for three particles. And less expectedly, our result stands in excellent agreement with the result of a hydrodynamic simulation (with the Lieb-Liniger equation of state as an input) of the microscopically large but macroscopically small excitations.We also show that the frequency we obtain coincides with the upper bound derived by Menotti and Stringari using sum rules. Surprisingly, however, we found that the usually successful hydrodynamic perturbation theory predicts a shift that is 9/4 higher than its ab initio numerical counterpart. We conjecture that the sharp boundary of the cloud in local density approximation—characterized by an infinite density gradient—renders the perturbation inapplicable. All our results also directly apply to the three-dimensional p-wave-interacting waveguide-confined fermions.
Recently, the quantum nature in the energy transport in solar cells and light-harvesting complexe... more Recently, the quantum nature in the energy transport in solar cells and light-harvesting complexes has attracted much attention as being triggered by the experimental observations. We model the light-harvesting complex (i.e., PEB50 dimer) as a quantum heat engine (QHE) and study the effect of the undamped intramolecule vibrational modes on the coherent energy-transfer process and quantum transport. We find that the exciton−vibration interaction has nontrivial contribution to the promotion of quantum yield as well as transport properties of the QHE at steady state by enhancing the quantum coherence quantified by entanglement entropy. The perfect quantum yield over 90% has been obtained, with the exciton−vibration coupling. We attribute these improvements to the renormalization of the electronic couplings effectively induced by exciton−vibration interaction and the subsequent delocalization of excitons. Finally, we demonstrate that the thermal relaxation and dephasing can help the excitation energy transfer in the PEB50 dimer.
Wedevelop a population and flux landscape theory for general non-equilibrium quantum systems. We ... more Wedevelop a population and flux landscape theory for general non-equilibrium quantum systems. We illustrate our theory by modelling the quantum transport of donor-acceptor energy transfer.We find two driving forces for the non-equilibrium quantum dynamics. The symmetric part of the driving force corresponds to the population landscape contribution which mainly governs the equilibrium part of dynamics while the anti-symmetric part of the driving force generates the non-equilibrium curl quantum flux which leads to the detailed-balance-breaking and time-irreversibility. The multiloop structure of the flux emerges forms the flux-landscape. Westudy the trend of changes in population and flux-landscape with respect to the voltage (temperature difference induced by environments) and electronic coupling. Improving the voltage and electronic coupling in general facilitates the quantum transport by reducing the population landscape barriers between major states and increasing the mean value of the flux. Alimit-cycle mode emerges when the underlying fluxlandscape becomes funnelled with a significant gap between the largest flux loop and the rest of them. On the kinetic level, we find that multiple kinetic paths between quantum states emerge and illustrate the interference effects. The degree of interference is determined by the landscape and flux. Furthermore, we quantify kinetic rate which strongly correlates with the population landscape and flux. For quantum transport, we demonstrate that as the coherence or the quantum entanglement is enhanced, the flux and energy transfer efficiency are increased. Finally it is surprising that the nonequilibriumness quantified by voltage has a non-trivial contribution on strengthening the entanglement, which is attributed to the non-local feature of the quantum curl flux.
We established a theoretical framework in terms of the curl flux, population landscape, and coher... more We established a theoretical framework in terms of the curl flux, population landscape, and coherence for non-equilibrium quantum systems at steady state, through exploring the energy and charge transport in molecular processes. The curl quantum flux plays the key role in determining transport properties and the system reaches equilibrium when flux vanishes. The novel curl quantum flux reflects the degree of non-equilibriumness and the time-irreversibility. We found an analytical expression for the quantum flux and its relationship to the environmental pumping (non-equilibriumness quantified by the voltage away from the equilibrium) and the quantum tunneling. Furthermore, we investigated another quantum signature, the coherence, quantitatively measured by the non-zero off
diagonal element of the density matrix. Populations of states give the probabilities of individual states and therefore quantify the population landscape. Both curl flux and coherence depend on steady state population landscape. Besides the environment-assistance which can give dramatic enhancement of coherence and quantum flux with high voltage at a fixed tunneling strength, the quantum flux is promoted by the coherence in the regime of small tunneling while reduced by the coherence in the regime of large tunneling, due to the non-monotonic relationship between the coherence and tunneling. This is in contrast to the previously found linear relationship. For the systems coupled to bosonic (photonic and phononic) reservoirs the flux is significantly promoted at large voltage while for fermionic (electronic) reservoirs the flux reaches a saturation after a significant enhancement at large voltage due to the Pauli exclusion principle. In view of the system as a quantum heat engine, we studied the non-equilibrium thermodynamics and established the analytical connections of curl quantum flux to the transport quantities such as energy (charge) transfer efficiency, chemical reaction
efficiency, energy dissipation, heat and electric currents observed in the experiments. We observed a perfect transfer efficiency in chemical reactions at high voltage (chemical potential difference). Our theoretical predicted behavior of the electric current with respect to the voltage is in good agreements with the recent experiments on electron transfer in single molecules.
In this article, we consider the monopole excitations of a harmonically trapped Bose gas in the v... more In this article, we consider the monopole excitations of a harmonically trapped Bose gas in the vicinity of the Tonks-Girardeau limit. Using Girardeau’s Fermi-Bose duality and subsequently an effective fermion-fermion odd-wave interaction, we obtain the dominant correction to the scale-invariance-protected value of the excitation frequency, for microscopically small excitation amplitudes. We produce a series of diffusion Monte Carlo results that confirm our analytic prediction for three particles. And less expectedly, our result stands in excellent agreement with the result of a hydrodynamic simulation (with the Lieb-Liniger equation of state as an input) of the microscopically large but macroscopically small excitations.We also show that the frequency we obtain coincides with the upper bound derived by Menotti and Stringari using sum rules. Surprisingly, however, we found that the usually successful hydrodynamic perturbation theory predicts a shift that is 9/4 higher than its ab initio numerical counterpart. We conjecture that the sharp boundary of the cloud in local density approximation—characterized by an infinite density gradient—renders the perturbation inapplicable. All our results also directly apply to the three-dimensional p-wave-interacting waveguide-confined fermions.
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Papers by Zhedong Zhang
diagonal element of the density matrix. Populations of states give the probabilities of individual states and therefore quantify the population landscape. Both curl flux and coherence depend on steady state population landscape. Besides the environment-assistance which can give dramatic enhancement of coherence and quantum flux with high voltage at a fixed tunneling strength, the quantum flux is promoted by the coherence in the regime of small tunneling while reduced by the coherence in the regime of large tunneling, due to the non-monotonic relationship between the coherence and tunneling. This is in contrast to the previously found linear relationship. For the systems coupled to bosonic (photonic and phononic) reservoirs the flux is significantly promoted at large voltage while for fermionic (electronic) reservoirs the flux reaches a saturation after a significant enhancement at large voltage due to the Pauli exclusion principle. In view of the system as a quantum heat engine, we studied the non-equilibrium thermodynamics and established the analytical connections of curl quantum flux to the transport quantities such as energy (charge) transfer efficiency, chemical reaction
efficiency, energy dissipation, heat and electric currents observed in the experiments. We observed a perfect transfer efficiency in chemical reactions at high voltage (chemical potential difference). Our theoretical predicted behavior of the electric current with respect to the voltage is in good agreements with the recent experiments on electron transfer in single molecules.
diagonal element of the density matrix. Populations of states give the probabilities of individual states and therefore quantify the population landscape. Both curl flux and coherence depend on steady state population landscape. Besides the environment-assistance which can give dramatic enhancement of coherence and quantum flux with high voltage at a fixed tunneling strength, the quantum flux is promoted by the coherence in the regime of small tunneling while reduced by the coherence in the regime of large tunneling, due to the non-monotonic relationship between the coherence and tunneling. This is in contrast to the previously found linear relationship. For the systems coupled to bosonic (photonic and phononic) reservoirs the flux is significantly promoted at large voltage while for fermionic (electronic) reservoirs the flux reaches a saturation after a significant enhancement at large voltage due to the Pauli exclusion principle. In view of the system as a quantum heat engine, we studied the non-equilibrium thermodynamics and established the analytical connections of curl quantum flux to the transport quantities such as energy (charge) transfer efficiency, chemical reaction
efficiency, energy dissipation, heat and electric currents observed in the experiments. We observed a perfect transfer efficiency in chemical reactions at high voltage (chemical potential difference). Our theoretical predicted behavior of the electric current with respect to the voltage is in good agreements with the recent experiments on electron transfer in single molecules.