Abstract
The response of the bacterial reaction center to entangled photons is com- pared with stochastic and chirped pulses. Nonlinear optical signals reveal how distribu- tions of exciton states may be controlled by quantum light.
Highlights
We show how frequency entanglement can be utilized to create exciton distributions in the bacterial reaction center B. viridis (Fig. 1A) that cannot be realized with classical pulses
The power spectra of the two beams may be very broad, the sum of their frequencies can still be sharply peaked due to the energy entanglement. This feature shows up in higher-order correlation functions, E†(t1)E†(t2)E(t4)E(t3), which determine third-order nonlinear signals
We have considered excitation by three types of light: entangled photon pairs, classical chirped pulses, and stochastic light all having the same spectral density
Summary
Quantum light provides novel possibilities for nonlinear spectroscopy by tuning parameters of the photon wavefunction. The energy-time entanglement can be used to control population transport in the single-exciton manifold, while the broad bandwidth of the two photons (Fig. 1B) allows to explore all the pathways through the single-exciton manifold (see Fig. 1C, [2]). These effects are clearly seen in two-photon-induced fluorescence signals. The simulations are based on a tight-binding formulation of the electronic Hamiltonian, and incorporate excitation energy transfer as well as the coupling to charge-separated states [3]
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