Tensor Network Simulation of Non-Markovian Dynamics in Organic Polaritons

Pino, Javier del; Schröder, Florian A. Y. N.; Chin, Alex W.; Feist, Johannes; García‐Vidal, F. J.

doi:10.1103/physrevlett.121.227401

Cited by 86 publications

(61 citation statements)

References 69 publications

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“…When this approximation is not applicable, more advanced numerical approaches such as tensor network calculations 47,48 or hierarchical equations of motion 49 can be employed, possibly after a chain transformation of the associated Hamiltonian 50 . Such approaches have been used to study static properties and dynamics in organic polaritons 51,52 . However, these are numerically demanding approaches that require significant computational resources.…”

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confidence: 99%

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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confidence: 99%

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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“…However, in contrast to the picture of Refs. 139,143,144 , here the cavity photon couples to the electronic excited state in the molecule, rather than to a transition, implying that the cavity photon actually shifts the manifold of excited state. Hence, the energies of the two polaritons (in the absence of heat baths and vibrations) should be ω L =ω e and ω U =ω e + ω c whereω e incorporates the vacuum Rabi frequency in the polariton frame.…”

Section: Cavity-induced Suppression Of Charge Currentmentioning

confidence: 97%

“…where κ ≡ F (ω c ) sets the bare cavity decay rate. For plasmonic cavities, we take κ = 0.05 eV 139 . From the initial vacuum state we get the nonvanishing correlation of the input field a in (t)a † in (t ) = dω F (ω) 2π 2 e −iω(t−t ) .…”

Section: Cavity-induced Suppression Of Charge Currentmentioning

confidence: 99%

“…To pinpoint the origin of these steps, we note that strong light-matter interaction can give rise to hybrid states, the so-called polariton states 141,142 . In analogy with the case where a cavity mode couples to an excitonic transition in molecules 139,143,144 , we expect that two hybrid states that correspond to the upper (U) and lower (L) polariton will form. However, in contrast to the picture of Refs.…”

Section: Cavity-induced Suppression Of Charge Currentmentioning

confidence: 99%

“…(55). The interplay between electron-vibration and light-matter interactions generates polariton states as a threefold mixture of photonic, electronic and phononic degrees of freedom 139,[145][146][147][148] , leading to the breakdown of the previous simple picture of two branches of polaritons. Hence, we observe more sophisticated step structures in Fig.…”

Section: Cavity-induced Suppression Of Charge Currentmentioning

confidence: 99%

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Generalized input-output method to quantum transport junctions. II. Applications

Liu

Segal

2020

Phys. Rev. B

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The interaction of electrons with atomic motion critically influences charge transport properties in molecular conducting junctions and quantum dot systems, and it is responsible for a plethora of transport phenomena. Nevertheless, theoretical tools are still limited to treat simple model junctions in specific parameter regimes. In this work, we put forward a generalized input-output method (GIOM) for studying charge transport in molecular junctions accounting for strong electron-vibration interactions and including electronic and phononic environments. The method radically expands the scope of the input-output theory, which was originally put forward to treat quantum optic problems. Based on the GIOM we derive a Langevin-type equation of motion for molecular operators, which posses a great generality and accuracy, and permits the derivation of a stationary charge current expression involving only two types of transfer rates. Furthermore, we devise the so-called "Polaron Transport in Electronic Resonance" (PoTER) approximation, which allows to feasibly simulate electron dynamics in generic tight-binding models with strong electron-vibration interactions. To illustrate the breadth of applications of the GIOM-PoTER technique, we analyze prototype molecular junction models with primary and secondary vibrational modes. For short chains, the charge current reduces to known limits and reasonably agrees with exact numerical simulations (when available). For extended junctions the current displays a turnover from phonon-assisted to phonon-suppressed transport. Nevertheless, the onset of ohmic behavior requires extensions beyond the PoTER approximation. As an additional application, we consider a cavity-coupled molecule junction. Here we identify a cavity-induced suppression of charge current in the single-site case, and observe signatures of polariton formation in the current-voltage characteristics in the strong light-matter coupling regime. A critical understanding gained from the GIOM-PoTER scheme is that the single-site vibrationally-coupled model is deceptively simpler, and amenable to approximations than multi-site models. Therefore, benchmarking of methods should not be concluded with the single-site case. The work manifests that the input-output framework, which is normally employed in quantum optics, can serve as a powerful and feasible tool in the realm of electron transport junctions.

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First Principles Modelling of Exciton-Photon Interactions

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2021

On Exciton–Vibration and Exciton–Photon Interactions in Organic Semiconductors

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Tensor Network Simulation of Non-Markovian Dynamics in Organic Polaritons

Cited by 86 publications

References 69 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

Generalized input-output method to quantum transport junctions. II. Applications

First Principles Modelling of Exciton-Photon Interactions

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