Critical phenomena and nonlinear dynamics in a spin ensemble strongly coupled to a cavity. II. Semiclassical-to-quantum boundary

Zens, Matthias; Krimer, Dmitry O.; Rotter, Stefan

doi:10.1103/physreva.100.013856

Cited by 20 publications

(23 citation statements)

References 53 publications

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“…Truncating this description by neglecting operator correlations above some order leads to a closed set of equations. This method was already applied in the context of cavity QED [56][57][58][59] , but a systematic study of the importance of the different terms appearing in the expansion has not been provided yet. We here present an extensive study of how different truncations of the cumulant expansion perform in the computation of the dynamics of the quantum emitter and EM modes.…”

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Cumulant expansion for the treatment of light–matter interactions in arbitrary material structures

Mónica

Silva

Feist

2020

The Journal of Chemical Physics

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Strong coupling of quantum emitters with confined electromagnetic modes of nanophotonic structures may be used to change optical, chemical and transport properties of materials, with significant theoretical effort invested towards a better understanding of this phenomenon. However, a full theoretical description of both matter and light is an extremely challenging task. Typical theoretical approaches simplify the description of the photonic environment by describing it as a single or few modes. While this approximation is accurate in some cases, it breaks down strongly in complex environments, such as within plasmonic nanocavities, and the electromagnetic environment must be fully taken into account. This requires the quantum description of a continuum of bosonic modes, a problem that is computationally hard. We here investigate a compromise where the quantum character of light is taken into account at modest computational cost. To do so, we focus on a quantum emitter that interacts with an arbitrary photonic spectral density and employ the cumulant or cluster expansion method to the Heisenberg equations of motion up to first, second and third order. We benchmark the method by comparing with exact solutions for specific situations and show that it can accurately represent dynamics for many parameter ranges.Light-matter interaction is of paramount importance for unraveling the laws of nature and its deep understanding allows us to control and manipulate physical and chemical systems. In particular, one can modify the properties of a quantum emitter simply by changing its electromagnetic environment, for example by enclosing it within an optical cavity. This may give rise to a change of the decay rate for spontaneous emission in the weak coupling regime, the so-called Purcell effect 1 , or to the appearance of hybrid light-matter states, socalled polaritons, in the strong-coupling regime 2-5 . Over the last decades, it has been shown that strong light-matter coupling can be achieved using a large variety of physical implementations as the "cavity" that provides the electromagnetic field confinement. These include Fabry-Perot cavities consisting of two mirrors 5 , propagating surface plasmon polaritons 6 , plasmonic hole 7 and nanoparticle arrays 8 , isolated plasmonic nanoparticles 9 and nanoparticle-on-mirror geometries 10,11 , as well as hybrid cavities combining plasmonic and dielectric materials [12][13][14] . In many of these systems, the electromagnetic field modes are not well-described by isolated lossy cavity modes, and a correct treatment demands theoretical approaches that are able to deal with the complexity of the electromagnetic field modes and their spectrum.In principle, to treat the problem of light-matter interaction, one can rely on the most general theory that describes light and matter on equal footing, i.e., quantum electrodynamics (QED) 15 . However, treating all light and matter degrees of freedom in the systems described above in a quantum mechanical way is an intractable problem and approx...

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Cumulant expansion for the treatment of light–matter interactions in arbitrary material structures

Mónica

Silva

Feist

2020

The Journal of Chemical Physics

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“…Note that (1) does not include direct dipole-dipole interactions, whichalthough present in the actual sample-do not seem to play a fundamental role for the formation of the echo pulses in our model. For large spin ensembles, we can use a mean-field formulation in the form of the Maxwell-Bloch equations for the resonator and spin expectation values [25,69],…”

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Echo Trains in Pulsed Electron Spin Resonance of a Strongly Coupled Spin Ensemble

et al. 2020

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“…Lindblad master equation(LME), the N TLSs in an optical cavity with light-matter coupling strength g, a driving laser with a Gaussian pulse envelope and peak amplitude 0 , and three decay channels corresponding to the cavity decay ( ), TLS dephasing ( ), and TLS relaxation ( − ). To solve this many-body LME, we make use of the cumulant expansion[29][30][31] , with model parameters given by a chi-squared minimisation of the experimental data. Experimental uncertainties are estimated from the point-to-point variance of the data.…”

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An organic quantum battery

Quach

McGhee

Ganzer

et al. 2020

Preprint

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Quantum batteries harness the unique properties of quantum mechanics to enhance energy storage compared to conventional batteries. In particular, they are predicted to undergo superextensive charging, where batteries with larger capacity actually take less time to charge. Up until now however, they have not been experimentally demonstrated, due to the challenges in quantum coherent control. Here we implement an array of two-level systems coupled to a photonic mode to realise a Dicke quantum battery. Our quantum battery is constructed with a microcavity formed by two dielectric mirrors enclosing a thin ﬁlm of a fluorescent molecular dye in a polymer matrix. We use ultrafast optical spectroscopy to time resolve the charging dynamics of the quantum battery at femtosecond resolution. We experimentally demonstrate superextensive increases in both charging power and storage capacity, in agreement with our theoretical modelling. We find that decoherence plays an important role in stabilising energy storage, analogous to the role that dissipation plays in photosynthesis. This experimental proof-of-concept is a major milestone towards the practical application of quantum batteries in quantum and conventional devices. Our work opens new opportunities for harnessing collective effects in light-matter coupling for nanoscale energy capture, storage, and transport technologies, including the enhancement of solar cell efficiencies.

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Critical phenomena and nonlinear dynamics in a spin ensemble strongly coupled to a cavity. II. Semiclassical-to-quantum boundary

Cited by 20 publications

References 53 publications

Cumulant expansion for the treatment of light–matter interactions in arbitrary material structures

Cumulant expansion for the treatment of light–matter interactions in arbitrary material structures

Echo Trains in Pulsed Electron Spin Resonance of a Strongly Coupled Spin Ensemble

An organic quantum battery

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