Optical signatures of electron-phonon decoupling due to strong light-matter interactions

Denning, Emil Vosmar; Bundgaard-Nielsen, Matias; Mørk, Jesper

doi:10.1103/physrevb.102.235303

Cited by 24 publications

(36 citation statements)

References 67 publications

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“…[ 54 ] Because we neglect the non‐Markovian effects, we also do not describe the acoustic phonon sideband, which in GaAs dots is about three orders of magnitudes below the Mollow triplet peaks. [ 58,59 ] Also for more evolved photon properties [ 60,61 ] or entangled photons, [ 62,63 ] the rate equations might fail depending on the parameter regime. Nonetheless, to describe the quantum dynamics of the electronic states in a QD, rate equations capture the essential features given that a non‐monotoneous phonon spectral density is taken into account and by their simplicity offer beautiful insight in the underlying physics.…”

Section: Dynamicsmentioning

confidence: 99%

Optical Signals to Monitor the Dynamics of Phonon‐Modified Rabi Oscillations in a Quantum Dot

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Reiter

2021

Annalen der Physik

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Semiconductor quantum dots are solid state few‐level systems which can interact strongly with light. As such, they can be used as a single photon source or to perform solid‐state quantum‐optics experiments. A major difference to atoms is the interaction with the lattice vibrations, that is, the phonons, which strongly affect the optical signals from a quantum dot. In this paper, we calculate the time‐resolved pump‐probe signals from a continuously driven quantum dot accounting for detuned excitation and electron–phonon interaction. We provide analytical equations giving insight into the different phenomena observed in the spectra like an oscillation between absorptive and dispersive line shapes. For detuned excitation, the electron–phonon interaction can lead to phonon‐assisted occupation of the exciton, giving rise to a strong asymmetry in the dynamical behavior depending on the sign of the detuning. The time‐resolved spectra monitor this relaxation path, which helps understanding the effect of electron–phonon interaction in quantum dots.

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Section: Dynamicsmentioning

confidence: 99%

Optical Signals to Monitor the Dynamics of Phonon‐Modified Rabi Oscillations in a Quantum Dot

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Reiter

2021

Annalen der Physik

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“…In this section, we present the underlying unitary transformations and derive the corresponding master equations. The unitary transformations considered are the identity transformation, the standard polaron transformation [38,44,[47][48][49], a variationally optimized polaron transformation [14,[50][51][52][53], and a polariton-polaron transformation. An illustration of the exciton-cavity-phonon system together with the effects of the variational polaron transformation and polariton-polaron transformation can be seen in Fig.…”

Section: Perturbative Master Equationsmentioning

confidence: 99%

“…Here, the strong emitter-cavity interaction can significantly influence and, in some cases, decouple the vibrational dynamics [11][12][13]. In this regime, the optical emission spectrum exhibits two distinct polariton peaks which are both dressed * mabuni1998@gmail.com with a distinct vibrational sideband [14,15]. On the other hand, resonant phonon-induced transitions between the polariton states is a dominating effect in the intermediate regime, where the polariton splitting is comparable with the typical environmental phonon frequency.…”

Section: Introductionmentioning

confidence: 99%

“…In this paper, we have implemented a computationally efficient tensor network formulation, which allows us to calculate two-time averages to any desired numerical precision [14,36,37]. These calculations are then used as a benchmark to evaluate the accuracy of various less complex and less computationally demanding and more physically intuitive perturbative master equations across a large range of light-matter coupling strengths.…”

Section: Introductionmentioning

confidence: 99%

“…The polariton-polaron approach is found to be the most accurate method in the strong-coupling regime, where phonons manifest themselves as sidebands on the polariton peaks [14,15]. The variational approach is, on the other hand, found to be precise in the Purcell regime, where the zero-phonon line acquires a phonon sideband [2,43].…”

Section: Introductionmentioning

confidence: 99%

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Non-Markovian perturbation theories for phonon effects in strong-coupling cavity quantum electrodynamics

2021

Self Cite

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Phonon interactions are inevitable in cavity quantum electrodynamical systems based on solid-state emitters or fluorescent molecules, where vibrations of the lattice or chemical bonds couple to the electronic degrees of freedom. Due to the non-Markovian response of the vibrational environment, it remains a significant theoretical challenge to describe such effects in a computationally efficient manner. This is particularly pronounced when the emitter-cavity coupling is comparable with or larger than the typical phonon energy range, and polariton formation coincides with vibrational dressing of the optical transitions. In this paper, we consider four non-Markovian perturbative master equation approaches to describe such dynamics over a broad range of light-matter coupling strengths and compare them with numerically exact reference calculations using a tensor network. The master equations are derived using different basis transformations, and a perturbative expansion in the transformed basis is subsequently introduced and analyzed. We find that two approaches are particularly successful and robust. The first of these is suggested and developed in this paper and is based on a vibrational dressing of the exciton-cavity polaritons. This enables the description of distinct phonon-polariton sidebands that appear when the polariton splitting exceeds the typical phonon frequency scale in the environment. The second approach is based on a variationally optimized polaronic vibrational dressing of the electronic state. Both of these approaches demonstrate good qualitative and quantitative agreement with reference calculations of the emission spectrum and are numerically robust, even at elevated temperatures, where the thermal phonon population is significant.

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Influence of Strong Molecular Vibrations on Decoherence of Molecular Polaritons

Rouse,

Gauger,

Lovett

2024

ACS Photonics

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We derive the transition rates, dephasing rates, and Lamb shifts for a system consisting of many molecules collectively coupled to a resonant cavity mode. Using a variational polaron master equation, we show that strong vibrational interactions inherent to molecules give rise to multi-phonon processes and suppress the light−matter coupling. In the strong light−matter coupling limit, multiphonon contributions to the transition and dephasing rates strongly dominate over single-phonon contributions for typical molecular parameters. This leads to novel dependencies of the rates and spectral line widths on the number of molecules in the cavity. We also find that vibrational Lamb shifts can substantially modify the polariton energies in the strong light−matter coupling limit.

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Optical signatures of electron-phonon decoupling due to strong light-matter interactions

Cited by 24 publications

References 67 publications

Optical Signals to Monitor the Dynamics of Phonon‐Modified Rabi Oscillations in a Quantum Dot

Optical Signals to Monitor the Dynamics of Phonon‐Modified Rabi Oscillations in a Quantum Dot

Non-Markovian perturbation theories for phonon effects in strong-coupling cavity quantum electrodynamics

Influence of Strong Molecular Vibrations on Decoherence of Molecular Polaritons

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