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Generation of Transient Quantum Coherence Using Partially Coherent Radiation

Z. S. Sadeq

Published Nov 26, 2012• 0 citations
OpenAlex

Abstract

We investigate quantum coherences between excited states induced on quantum systems upon excitation by partially coherent radiation sources. Attempts at rejuvenating coherences using noisy sources are also explored. This work is most relevant to studies of photo-excitation of light harvesting systems under natural conditions as well as to quantum optical experiments using partially coherent lasers. The transient coherent response of a model $V$ system upon irradiation by various models of incoherent light is explored and it was found that it was possible to induce transient excited state coherences upon excitation. These excited state coherences eventually become a small fraction of population and the system reaches a mixed state. Lastly, we critique an existing literature model of excitation by noisy laser and we show that the coherence observed in that scenario is artificial. We propose an alternative using a physical model of noisy excitation.

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We investigate quantum coherences between excited states induced on quantum systems upon excitation by partially coherent radiation sources. Attempts at rejuvenating coherences using noisy sources are also explored. This work is most relevant to studies of photo-excitation of light harvesting systems under natural conditions as well as to quantum optical experiments using partially coherent lasers. The transient coherent response of a model VVV system upon irradiation by various models of incoherent light is explored and it was found that it was possible to induce transient excited state coherences upon excitation. These excited state coherences eventually become a small fraction of population and the system reaches a mixed state. Lastly, we critique an existing literature model of excitation by noisy laser and we show that the coherence observed in that scenario is artificial. We propose an alternative using a physical model of noisy excitation.
The response of an arbitrary closed quantum system to a partially coherent electric field is investigated, with a focus on the transient coherences in the system. As a model we examine, both perturbatively and numerically, the coherences induced in a three level V system. Both rapid turn-on and pulsed turn-on effects are investigated. The effect of a long and incoherent pulse is also considered, demonstrating that during the pulse the system shows a coherent response which reduces after the pulse is over. Both the pulsed scenario and the thermally broadened CW case approach a mixed state in the long time limit, with rates dictated by the adjacent level spacings and the coherence time of the light, and via a mechanism that is distinctly different from traditional decoherence. These two excitation scenarios are also explored for a minimal "toy" model of the electronic levels in pigment protein complex PC645 by both a collisionally broadened CW laser and by a noisy pulse, where unexpectedly long transient coherence times are observed and explained. The significance of environmentally induced decoherence is noted.
Abstract Excitation of molecules by incident incoherent electromagnetic radiation, such as sunlight, is described in detail and contrasted with the effect of coherent (e.g. laser) light. The nature of the quantum coherences induced by the former, relevant to transport processes in nature and in technology, is emphasized. Both equilibrium and steady state scenarios are discussed, three examples: simple models, calcium excitation in polarized light, and the isomerization of retinal in rhodopsin are used to expose the underlying qualitative nature of the established coherences.
Optical response of an active medium can substantially be modified when coherent superpositions of states are excited, that is, when systems display quantum coherence and interference. This has led to fascinating applications in atomic and molecular systems. Examples include coherent population trapping, lasing without inversion, electromagnetically induced transparency, cooperative spontaneous emission, and quantum entanglement. \n \nWe study quantum coherence effects in several quantum optical systems and find interesting applications. We show that quantum coherence can lead to transient Raman lasing and lasing without inversion in short wavelength spectral regions--extreme ultraviolet and x-ray--without the requirement of incoherent pumping. For example, we demonstrate transient Raman lasing at 58.4 nm in Helium atom and transient lasing without inversion at 6.1 nm in Helium-like Boron (triply-ionized Boron). We also investigate dynamical properties of a collective superradiant state prepared by absorption of a single photon when the size of the sample is larger than the radiation wavelength. We show that for large number of atoms such a state, to a good approximation, decays exponentially with a rate proportional to the number of atoms. We also find that the collective frequency shift resulting from repeated emission and reabsorption of short-lived virtual photons is proportional to the number of species in the sample. Furthermore, we examine how a position-dependent excitation phase affects the evolution of entanglement between two dipole-coupled qubits. It turns out that the coherence induced by position-dependent excitation phase slows down the otherwise fast decay of the two-qubit entanglement. We also show that it is possible to entangle two spatially separated and uncoupled qubits via interaction with correlated photons in a cavity quantum electrodynamics setup. Finally, we analyze how quantum coherence can be used to generate continuous-variable entanglement in quantum-beat lasers in steady state and propose possible implementation in quantum lithography.
The excitation of molecular systems by incoherent light is studied primarily using a V-system model in the Partial Secular Bloch-Redfield formalism. First, the dynamical regimes are characterized for a system irradiated by suddenly turned on light and the relevant timescales are defined in terms of system parameters. Then excitation by slowly turned-on light is studied, showing a decay in the magnitude of noise-induced coherences with increasing turn-on times, leading to their disapearance in the very slow turn-on limit relevant to many natural systems.
Dynamics and coherences in retinal isomerization are investigated in a standard two-mode two-state model irradiated by natural incoherent light using the Markovian partial-secular Bloch-Redfield formalism. The two-mode two-state model is a minimal model of retinal that considers vibronic states on a ground and excited electronic manifold coupled to two continuous Ohmic harmonic baths. All light-induced coherent oscillations are shown to disappear as the turn-on time becomes realistically slow. Rather, an interplay between incoherent-light induced coherences and environmentally induced coherences is exposed as the system approaches a nonequilibrium steady state. The dynamics of the system reveal stable steady state coherences under realistic conditions, producing a small but robust transient enhancement of quantum yield.
We present an efficient theoretical method for calculating the time evolution of the density matrix of a multilevel quantum system weakly interacting with incoherent light. The method combines the Bloch-Redfield theory with a partial secular approximation for one-photon coherences, resulting in a master equation that explicitly exposes the reliance on transition rates and the angles between transition dipole moments in the energy basis. The partial secular Bloch-Redfield master equation allows an unambiguous distinction between the regimes of quantum coherent vs. incoherent energy transfer under incoherent light illumination. The fully incoherent regime is characterized by orthogonal transition dipole moments in the energy basis, leading to a dynamical evolution governed by a coherence-free Pauli-type master equation. The coherent regime requires non-orthogonal transition dipole moments in the energy basis and leads to the generation of noise-induced quantum coherences and population-to-coherence couplings. As a first application, we consider the dynamics of excited state coherences arising under incoherent light excitation from a single ground state and observe population-to-coherence transfer and the formation of non-equilibrium quasisteady states in the regime of small excited state splitting. Analytical expressions derived earlier for the V-type system [T. V. Tscherbul and P. Brumer, Phys. Rev. Lett. 113, 113601 (2014)] are found to provide a nearly quantitative description of multilevel excited-state populations and coherences in both the small- and large-molecule limits.