Microcavity phonon polaritons from the weak to the ultrastrong phonon–photon coupling regime

Barra-Burillo, María; Muniain, Unai; Catalano, Sara; Autore, Marta; Casanova, Fèlix; Hueso, Luis E.; Aizpurua, Javier; Esteban, Rubén; Hillenbrand, Rainer

doi:10.1038/s41467-021-26060-x

Cited by 34 publications

(35 citation statements)

References 72 publications

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“…The maximum splitting that can be reached for a given material turns out to be the well-known value obtained for bulk polaritons, 66 and is independent of cavity geometry. 64 , 65 , 67 , 68 …”

Section: Overview Of Experimental Setupsmentioning

confidence: 99%

Theoretical Challenges in Polaritonic Chemistry

2022

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Polaritonic chemistry exploits strong light–matter coupling between molecules and confined electromagnetic field modes to enable new chemical reactivities. In systems displaying this functionality, the choice of the cavity determines both the confinement of the electromagnetic field and the number of molecules that are involved in the process. While in wavelength-scale optical cavities the light–matter interaction is ruled by collective effects, plasmonic subwavelength nanocavities allow even single molecules to reach strong coupling. Due to these very distinct situations, a multiscale theoretical toolbox is then required to explore the rich phenomenology of polaritonic chemistry. Within this framework, each component of the system (molecules and electromagnetic modes) needs to be treated in sufficient detail to obtain reliable results. Starting from the very general aspects of light–molecule interactions in typical experimental setups, we underline the basic concepts that should be taken into account when operating in this new area of research. Building on these considerations, we then provide a map of the theoretical tools already available to tackle chemical applications of molecular polaritons at different scales. Throughout the discussion, we draw attention to both the successes and the challenges still ahead in the theoretical description of polaritonic chemistry.

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Section: Overview Of Experimental Setupsmentioning

confidence: 99%

Theoretical Challenges in Polaritonic Chemistry

2022

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“…Since the driving field is weak enough, the hybrid system will stay at the ground state with almost 1 probability, which can be explicitly illustrated by the populations of the lower 9 eigenstates plotted in Fig. 3, where all the parameters are selected within the current experimental conditions [35,63]. Note that the population |C j | 2 at ω d ≈ 1.05ω 0 is about two order of the magnitude less than the population |C 1 | 2 at ω d ≈ 0.74ω 0 in Fig.…”

Section: Parity-conserving Casementioning

confidence: 99%

Photon and phonon statistics in a qubit-plasmon-phonon ultrastrong coupling system

Ma,

Horoshko,

et al. 2022

Preprint

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We study photon/phonon statistics of a qubit-plasmon-phonon hybrid system in the ultrastrong coupling regime. The introduced qubit coupling causes parity conserving and non-conserving situations. We employ an analytic approximation approach for the parity conserving case to reveal the statistical behaviors of photons and phonons. It indicates that both photons and phonons show strong antibunching at the same frequency. Even though the bunching properties of photons/phonons occupy the dominant regions of the considered frequencies, phonons tend to weakly antibunching within the photonic strong-bunching area. In contrast, one can find that the configurations of correlation functions for both photons and phonons in the parity conserving case are squeezed towards the central frequency by parity breaking, which directly triggers the reverse statistical behaviors for the different parties at the low-frequency regions and the strong bunching properties at other frequency regions. The photon-phonon cross-correlation function also demonstrates similar parity-induced differences, indicating that the non-conserving parity induces the photon-phonon bunching behavior. We finally analyze the delayed second-order correlation function with different driving frequencies, which illustrates striking oscillations revealing the occurrence of simultaneous multiple excitations.

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“…The plasmon then exchanges energy with the phonon mode of the silica slab through electromagnetic coupling. The equation of motion of the system is described by a linear differential equation system 55 − 58 ( Supporting Information section 6 ). The steady-state solution for the displacement of the driven oscillator gives the polarization induced by the plasmon excitation P = e x and can be written as where Γ j = ω j 2 – iγ j ω – ω 2 is the frequency-dependent response of each oscillator and K = 2 giω is the coupling term.…”

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confidence: 99%

“…The result of η = 0.13 > 0.1 shows that the hybridization between propagating nanotube Luttinger-liquid plasmons and silica phonons reaches the ultrastrong coupling regime; 59 thus, the damping can be neglected when calculating the eigenfrequencies. While eq 1 is an approximation for the eigenfrequencies, in this case we can formulate the exact solution as 17 , 58 Dispersion curves calculated this way are displayed in Figure 3 b as red dashed lines. They align well with the maxima of the theoretical dispersion map.…”

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confidence: 99%

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Direct Visualization of Ultrastrong Coupling between Luttinger-Liquid Plasmons and Phonon Polaritons

et al. 2022

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Ultrastrong coupling of light and matter creates new opportunities to modify chemical reactions or develop novel nanoscale devices. One-dimensional Luttinger-liquid plasmons in metallic carbon nanotubes are long-lived excitations with extreme electromagnetic field confinement. They are promising candidates to realize strong or even ultrastrong coupling at infrared frequencies. We applied near-field polariton interferometry to examine the interaction between propagating Luttinger-liquid plasmons in individual carbon nanotubes and surface phonon polaritons of silica and hexagonal boron nitride. We extracted the dispersion relation of the hybrid Luttinger-liquid plasmon–phonon polaritons (LPPhPs) and explained the observed phenomena by the coupled harmonic oscillator model. The dispersion shows pronounced mode splitting, and the obtained value for the normalized coupling strength shows we reached the ultrastrong coupling regime with both native silica and hBN phonons. Our findings predict future applications to exploit the extraordinary properties of carbon nanotube plasmons, ranging from nanoscale plasmonic circuits to ultrasensitive molecular sensing.

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Microcavity phonon polaritons from the weak to the ultrastrong phonon–photon coupling regime

Cited by 34 publications

References 72 publications

Theoretical Challenges in Polaritonic Chemistry

Theoretical Challenges in Polaritonic Chemistry

Photon and phonon statistics in a qubit-plasmon-phonon ultrastrong coupling system

Direct Visualization of Ultrastrong Coupling between Luttinger-Liquid Plasmons and Phonon Polaritons

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