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The Journal of Chemical Physics

Many-photon excitation of organic molecules in a cavity—Superradiance as a measure of coherence

Inga S. Ulusoy, Johana A. Gómez, Oriol Vendrell

Published Dec 23, 2020• 12 citations
Publisher

Abstract

Coherent excitation of a molecular ensemble coupled to a common radiation mode can lead to the collective emission of radiation known as superradiance. This collective emission only occurs if there is an entanglement between the molecules in their ground and excited state and can, therefore, serve as a macroscopic measure of coherence in the ensemble. Reported here are wave packet propagations for various pyrazine models of increasing complexity and molecular ensembles thereof. We show that ensemble coherence upon photoexcitation can prevail up to relatively long time scales although the effect can diminish quickly with increasing ensemble size. Coherence can also build up over time and even reemerge after the molecules have passed through a conical intersection. The effect of the pump pulse characteristics on the collective response of the molecular ensemble is also studied. A broadband pulse imprints a large amount of initial coherence to the system, as compared to a longer pulse with a smaller spread in the frequency domain. However, the differential effects arising from a different pulse duration and coherent bandwidth become less prominent if the emission of light from the ensemble takes place after a non-adiabatic decay process.

DOI
10.1063/5.0034786

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Coherent excitation of a molecular ensemble coupled to a common radiation mode can lead to the collective emission of radiation known as superradiance. This collective emission only occurs if there is an entanglement between the molecules in their ground and excited state and can, therefore, serve as a macroscopic measure of coherence in the ensemble. Reported here are wave packet propagations for various pyrazine models of increasing complexity and molecular ensembles thereof. We show that ensemble coherence upon photoexcitation can prevail up to relatively long time scales although the effect can diminish quickly with increasing ensemble size. Coherence can also build up over time and even reemerge after the molecules have passed through a conical intersection. The effect of the pump pulse characteristics on the collective response of the molecular ensemble is also studied. A broadband pulse imprints a large amount of initial coherence to the system, as compared to a longer pulse with a smaller spread in the frequency domain. However, the differential effects arising from a different pulse duration and coherent bandwidth become less prominent if the emission of light from the ensemble takes place after a non-adiabatic decay process.
The dynamical evolution of an excited-state population in a macroscopic volume of three-level molecules is considered where the population is driven optically between the initial ground state and the excited states by an externally applied (ccc-number) coherent pump. The intermediate and ground states are taken as nonradiatively coupled whereas the excited-to-intermediate-state transition is coupled to the radiation field which is treated quantum mechanically. It is found that stimulated Raman processes can significantly influence the dynamical evolution of population inversion and macroscopic polarization by producing coherence effects among the populations. We examine the evolution of collective relaxation between the excited and intermediate levels in the time regime of the pump pulse duration. It is shown, using the mean-field approximation, that for uniform pumping and conditions such that the pump Rabi rate ${\ensuremath{\omega}}_{R}$, the characteristic collective radiation time ${\ensuremath{\tau}}_{R}$, and the pump pulse duration ${\ensuremath{\tau}}_{P}$ satisfy the inequalities, ${\ensuremath{\omega}}_{R}>\frac{1}{{\ensuremath{\tau}}_{R}}>\ensuremath{\gamma}$ and ${\ensuremath{\tau}}_{P}\ensuremath{\gtrsim}{\ensuremath{\tau}}_{R}$ ($\ensuremath{\gamma}$ is a characteristic internal dephasing rate for the molecules), the system is left in a state with classical transverse polarization when the pump pulse terminates. The system can evolve collectively from such a state only as superradiant (classical) evolution. For superfluorescent evolution which requires a state of preparation of complete inversion (zero transverse polarization), it is shown that the pump pulse must be effectively of area $\ensuremath{\pi}$ and that ${\ensuremath{\tau}}_{P}<{\ensuremath{\tau}}_{R}$. Our results show that when the former conditions are satisfied the delay time ${\ensuremath{\tau}}_{D}$ for collective free pulse evolution is a function of both ${\ensuremath{\tau}}_{P}$ and ${\ensuremath{\tau}}_{R}$. It is shown further that the pump pulse shape as well as temporal duration significantly affect the final state of preparation. The results of this work are interpreted in connection with recent reported results of experiments in superfluorescence and superradiance.
The formalism of collective (Dicke-like) states and operators is used to describe the relaxation of the initially prepared state of a material in the presence of a laser field. The material states are shown to be expressible as minimum uncertainty wave packets formed from those special collective states that couple with the radiation field. It is shown that these coherent states of matter exhibit all the features that are usually attributed to ensemble averages of two-level molecules in a conventional statistical picture. However, there are new features in the quantum mechanical model when there are correlations among the molecules in the ensemble. The loss of minimum uncertainty characteristics of the wave packet correspnds to the transverse (T2) relaxation of the statistical model. Different types of T2 processes can be defined corresponding to the decay of different orders of coherence of the wave packet. Only for the case that the system decays in all orders of coherence do the quantum and statistical results coincide. There is expected to be a transverse relaxation that preserves one or more orders of coherence. Experiments are suggested that can test these ideas. A particular case of the formalism of collective states applies to molecular crystals and it provides a quantum mechanical picture of the dephasing of molecular excitons in terms of orders of coherence analogous to the usual manner of describing states of the radiation field.
Free induction decay is the coherent emission of light that follows the excitation of a medium by a short pulse. During the coherence time of the medium (T2), all atoms/molecules oscillate ’in unison’, forming a macroscopic dipole that emits light as a large coherent antenna, ’broadcasting’ information on the quantum state of the atoms/molecules and its dynamical evolution. We present an optical oscillator, where the coherent dipole emission from a dynamical wave-packet, is amplified beyond the lasing threshold. By placing a molecular medium in an optical cavity that is synchronously pumped by a frequency comb laser, emission from the excitation of one pump pulse can return to the medium with subsequent pump pulses, allowing stimulated amplification. When threshold is crossed, a broadband coherent oscillation is achieved, bearing information on the coherent wave-packet dynamics inside the medium. We analyze theoretically this coherent Raman oscillator and simulate thoroughly it’s dynamics under most realistic conditions for a model system of Alkali dimers (Li2,K2) in a hot gas cell (100−300 ◦ C), showing that the oscillation condition is well within reach. If realized, this coherent Raman oscillator can open avenues for precise measurement of vibrational dynamics in molecules.
When a quantum system is put into an excited state, it will decay back to the ground state through a process termed spontaneous emission.It is generally assumed that spontaneous emissions between different individual emitters will not be coherent with each other; to produce coherent light, one would need population inversion and stimulated emission.In this work, we show that an optically thin ensemble of 11 000 radiating atoms spontaneously organizes to produce spatially coherent light.The reason for this coherence is collective coupling of the individual emitters via Dicke superradiance and subradiance (as opposed to amplification through stimulated emission).
Superradiance is an extensive cooperative spontaneous emission phenomenon, exhibited by some atomic collective-spin states. However, distinct initial states differ in their decay dynamics. Dicke states ∣j,m⟩|j,m\rangle∣j,m⟩ with distinct numbers of excitations n=m+jn=m+jn=m+j, driven by vacuum fluctuations, have their peak emission intensity shifted in time. Rotating Dicke states relative to the decay axis introduces an interesting parity structure that affects the pulse profile and photon correlations. Squeezed-bath prepared states undergo a squeezing-controlled crossover to the rotated Dicke states, making the emission character dependent on the amount of squeezing transferred from light to the atomic state. For semiclassical states with a macroscopic dipole moment, like the atomic coherent state, the emission intensity depends on their polarization. We present detailed results on the superradiant dynamics of a representative selection of states expanded in Dicke states to highlight the initial state as an independent dynamical control parameter. For large-NNN, we are able to predict fairly accurately the pulse profile in each case using the mean-field approximation, an approach based on the Fokker--Planck equation. We also present comparative results on the intensity correlation function, quantify the coherent and incoherent contributions of the emission, and contrast between small and large ensembles.
Superradiance in an ensemble of atoms leads to the collective enhancement of radiation in a particular mode shared by the atoms in their spontaneous decay from an excited state. The quantum aspects of this phenomenon are highlighted when such collective enhancement is observed in the emission of a single quantum of light. Here we report a further step in exploring experimentally the nonclassical features of superradiance by implementing the process not only with single excitations, but also in a two-excitation state. Particularly, we measure and theoretically model the wave packets corresponding to superradiance in both the single-photon and two-photon regimes. Such progress opens the way to the study and future control of the interaction of nonclassical light modes with collective quantum memories at higher photon numbers.