Kubo-Anderson theory of polariton line shape

Climent, Clàudia; Subotnik, Joseph E.; Nitzan, Abraham

doi:10.1103/physreva.109.052809

Cited by 4 publications

(6 citation statements)

References 56 publications

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“…As a result, the polariton linewidth scales as 1/N under the fast limit, which differs from the no narrowing effect prediction of Kubo-Anderson theory under the fast limit in Ref. 31. Note that the scaling relations with N in Eqs.…”

Section: The Fast Limitcontrasting

confidence: 70%

“…By solving the nonperturbative coupled equations of motion of the exciton and cavity photon system numerically, they successfully recovered the experimental results by Whittaker et al [14] in terms of motional narrowing, explaining both the subaverage behavior and why the upper UP is always broader than the LP -due to inter-branch scattering, in which the multiple scattering to all orders is emphasized [25]. Nevertheless, a lot of theoretical controversies are generated and remain unresolved [11,[25][26][27][28][29][30][31]. For example, it is mentioned in Ref.…”

Section: Introductionmentioning

confidence: 59%

“…Moreover, the linewidth scales as 1/ √ N as is exhibited in panel (f), which is expected according to Eq. 29b as well as the Kubo-Anderson theory [31]. Furthermore, the lineshape is almost symmetric for the UP and the LP branches, due to much weaker inter-branch scatterings.…”

Section: B Polariton Linewidth Scaling With Nmentioning

confidence: 72%

“…Recently, Climent, Subotnik, and Nitzan [31] applied the Kubo-Anderson classical stochastic theory of molecular spectral lineshape [32][33][34] to the case of polaritons formed in the collective strong coupling regime. By including only one cavity mode which collectively interacts with many molecules, they provided simple analytic results in the fast and slow limits of the disorder dynamics and can be evaluated numerically for the intermediate case.…”

Section: Introductionmentioning

confidence: 99%

“…31, we want to emphasize that the Kubo-Anderson theory is classical and Markovian. It predicts that no narrowing effect can be exhibited under the fast limit [31], and does not explain the experimentally observed asymmetry between the UP and LP linewidths. Moreover, Ref.…”

Section: Introductionmentioning

confidence: 99%

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Theory and Quantum Dynamics Simulations of Exciton-Polariton Motional Narrowing

Ying,

Mondal,

Huo

2024

Preprint

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The motional narrowing effect has been extensively studied for cavity exciton-polariton systems in recent decades both experimentally and theoretically, which is featured by (1) the subaverage behavior, and (2) the asymmetric linewidths for the upper polariton (UP) and the lower polariton (LP). However, a minimal theoretical model that is clear and adequate to address all these effects, as well as the linewidth scaling relations remains missing. In this work, based on the single mode 1D Holstein-Tavis-Cummings (HTC) model, we studied the motional narrowing effect of the polariton linear absorption (LA) spectra via both semi-analytic derivations and numerically exact quantum dynamics simulations using the hierarchical equations of motion (HEOM) approach. The results reveal that under collective light-matter coupling between a cavity mode and $N$ molecules, the polariton linewidth scales as $1/\sqrt{N}$ under the slow limit, while scales as $1/N$ under the fast limit, due to the polaron decoupling effect. Further, by varying the detunings, the polariton linewidths exhibit significant motional narrowing, covering both characters mentioned above. Our analytic linewidth expressions agree well with the numerical exact simulations in all the parameter regimes we explored. These results indicate that the physics of motional narrowing is adequately accounted for by the single-mode 1D HTC model. We envision that both the numerical results and the analytic polariton linewidths expression presented in this work will offer great theoretical value for providing a better understanding of the exciton-polariton motional narrowing based on the HTC model.

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Section: The Fast Limitcontrasting

confidence: 70%

Section: Introductionmentioning

confidence: 59%

Section: B Polariton Linewidth Scaling With Nmentioning

confidence: 72%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Theory and Quantum Dynamics Simulations of Exciton-Polariton Motional Narrowing

Ying,

Mondal,

Huo

2024

Preprint

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Optical Emission Spectra of Molecular Excitonic Polariton Computed at the First‐Principles Level QED‐TDDFT

Deng,

Yang,

Shao

et al. 2024

ChemPhotoChem

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In microcavity, strong coupling between light and molecules leads to the formation of hybrid excitations, i.e., the polaritons, or exciton‐polaritons. Such coupling may alter the energy landscape of the system and the optical properties of the material, making it an effective approach for controlling the light emission from molecular materials. However, due to the complexity of vibrational modes, spectroscopic calculations for organic exciton‐polaritons remain to be challenging. In this work, based on the linear‐response quantum‐electrodynamical time‐dependent density functional theory (QED‐TDDFT), we employ the thermal vibrational correlation function (TVCF) formalism to calculate the molecular optical spectrum of the lower polaritons (LP) at first‐principles level for three molecules, i.e., anthracene, distyrylbenzenes (DSB), and rubrene. The polaron decoupling effect is confirmed from our first‐principles computations. The theoretical emission spectra of LP provide fruitful insights for molecular and device design in microcavities that are otherwise hindered due to the lack of vibrational information.

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Theory and quantum dynamics simulations of exciton-polariton motional narrowing

Ying,

Mondal,

Huo

2024

The Journal of Chemical Physics

View full text Add to dashboard Cite

The motional narrowing effect has been extensively studied for cavity exciton–polariton systems in recent decades both experimentally and theoretically, which is featured by (1) the subaverage behavior and (2) the asymmetric linewidths for the upper polariton and the lower polariton. However, a minimal theoretical model that is clear and adequate to address all these effects as well as the linewidth scaling relations remains missing. In this work, based on the single mode 1D Holstein–Tavis–Cummings (HTC) model, we studied the motional narrowing effect of the polariton linear absorption spectra via both semi-analytic derivations and numerically exact quantum dynamics simulations using the hierarchical equations of motion approach. The results reveal that under collective light–matter coupling between a cavity mode and N molecules, the polariton linewidth scales as 1/N under the slow limit, while scales as 1/N under the fast limit, due to the polaron decoupling effect. Furthermore, by varying the detunings, the polariton linewidths exhibit significant motional narrowing, covering both characters mentioned above. Our analytic linewidth expressions [Eqs. (34) and (35)] agree well with the numerical exact simulations in all the parameter regimes we explored. These results indicate that the physics of motional narrowing is adequately accounted for by the single-mode 1D HTC model. We envision that both the numerical results and the analytic polariton linewidths expression presented in this work will offer great theoretical value for providing a better understanding of the exciton–polariton motional narrowing based on the HTC model.

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Kubo-Anderson theory of polariton line shape

Cited by 4 publications

References 56 publications

Theory and Quantum Dynamics Simulations of Exciton-Polariton Motional Narrowing

Theory and Quantum Dynamics Simulations of Exciton-Polariton Motional Narrowing

Optical Emission Spectra of Molecular Excitonic Polariton Computed at the First‐Principles Level QED‐TDDFT

Theory and quantum dynamics simulations of exciton-polariton motional narrowing

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