Zero-phonon lines of systems with different dimensions and unconventional vibronic interactions

Hizhnyakov, V.

doi:10.1088/0953-8984/24/10/104011

Cited by 7 publications

(6 citation statements)

References 43 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…5(a),(b) that linear Holstein coupling can consequently lead to a temperaturedependent zero-phonon line if there is a large density of low frequency (long wavelength) phonon modes with ω k < γ which is the case in 1D but not in higher dimensions. This peculiarity of dephasing in 1D has already been discussed in the literature [68,69,73]. It is however also well established within the literature that the major contribution of the experimentally observed broadening of the zero-phonon line is caused by a higher-order electron-phonon interaction of the form [70,[73][74][75]]…”

Section: Dephasingsupporting

confidence: 51%

“…In the continuum limit considered here, this spectral density would lead to a divergence of the integral in Eq. ( 24) due to the high density of low-frequency phonons, which is a well known problem for 1D crystals [68,69]. This issue can be resolved by considering only a finite-sized 1D crystal with a minimum phonon frequency ω min > 0.…”

Section: B Phonon Imprint On Spectramentioning

confidence: 99%

See 1 more Smart Citation

Molecule-photon interactions in phononic environments

Reitz,

Sommer,

Gurlek

et al. 2019

Preprint

View full text Add to dashboard Cite

Molecular spectroscopy in the solid-state crucially depends on the interaction of electronic degrees of freedom with a highly complex vibrational environment. The large number of intramolecular vibrations (vibrons) and crystal vibrations (phonons) have often reduced the analysis of these driven molecular systems to a limited set of vibrations and numerical studies. We describe the non-equilibrium dynamics of light-matter systems comprised of guest molecules hosted in crystalline environments including finite thermal occupancies of vibrons and phonons. Using an open-system approach based on quantum Langevin equations, we provide analytical expressions for absorption and emission spectra with arbitrary numbers of vibronic and phononic modes. Exploiting the potential of this framework, we find that vibron-phonon coupling leads to a generally non-Markovian vibrational relaxation dynamics and that the common coupling to phonons can mediate collective vibron-vibron interactions similar to the processes of sub-and superradiance for radiative transitions. For molecular polaritonic scenarios with a strongly confined quantum light mode, we analytically characterize the imprint of vibronic and phononic couplings onto the cavity transmission profile and derive effective polariton cross-talk rates for finite baths occupancies.

show abstract

Section: Dephasingsupporting

confidence: 51%

Section: B Phonon Imprint On Spectramentioning

confidence: 99%

Molecule-photon interactions in phononic environments

Reitz,

Sommer,

Gurlek

et al. 2019

Preprint

View full text Add to dashboard Cite

show abstract

“…2). Acceptable fitting could not be achieved by the conventional T 4 dependence but required additional T 2 term to take into account softening of bonds in the excited electronic state in accordance of a modified model of the ZPL of impurity centers in solids [4].…”

Section: Methodsmentioning

confidence: 99%

Room Temperature Optical Thermometry Based on the Luminescence of the SiV Defects in Diamond

et al. 2019

View full text Add to dashboard Cite

SiV-containing microcrystals of diamond are synthesised by using high-pressure high-temperature treatment of a mixture of pertinent organic-inorganic precursors. Photoluminescence of SiV defects were investigated with the aim to use the microcrystals for optical temperature sensing in near infrared at room temperature based on temperaturedependent shift of the 740 nm zero-phonon line of SiV photoemission.

show abstract

“…5(a) and 5(b), we can see that linear Holstein coupling can consequently lead to a temperaturedependent zero-phonon line if there is a large density of low frequency (long wavelength) phonon modes with ω k < γ which is the case in 1D but not in higher dimensions. This peculiarity of dephasing in 1D has already been discussed in the literature [49,50,54]. It is however also well established within the literature that the major contribution of the experimentally observed temperature-dependent broadening of the zero-phonon line is caused by a higher-order electron-phonon interaction of the form [51,[54][55][56]]…”

Section: Dephasingmentioning

confidence: 53%

“…In the continuum limit considered here, this spectral density would lead to a divergence of the integral in Eq. (24) due to the high density of low-frequency phonons, which is a well known problem for 1D crystals [49,50]. This issue can be addressed by considering only a finite-sized 1D crystal with a minimum phonon frequency cutoff ω min > 0.…”

Section: B Phonon Imprint On Spectramentioning

confidence: 99%

Molecule-photon interactions in phononic environments

Reitz

Sommer

Gurlek

et al. 2020

Phys. Rev. Research

View full text Add to dashboard Cite

Molecules constitute compact hybrid quantum optical systems that can interface photons, electronic degrees of freedom, localized mechanical vibrations, and phonons. In particular, the strong vibronic interaction between electrons and nuclear motion in a molecule resembles the optomechanical radiation pressure Hamiltonian. While molecular vibrations are often in the ground state even at elevated temperatures, one still needs to get a handle on decoherence channels associated with phonons before an efficient quantum optical network based on optovibrational interactions in solid-state molecular systems could be realized. As a step towards a better understanding of decoherence in phononic environments, we take here an open quantum system approach to the nonequilibrium dynamics of guest molecules embedded in a crystal, identifying regimes of Markovian versus non-Markovian vibrational relaxation. A stochastic treatment, based on quantum Langevin equations, predicts collective vibron-vibron dynamics that resembles processes of sub-and super-radiance for radiative transitions. This in turn leads to the possibility of decoupling intramolecular vibrations from the phononic bath, allowing for enhanced coherence times of collective vibrations. For molecular polaritonics in strongly confined geometries, we also show that the imprint of optovibrational couplings onto the emerging output field results in effective polariton cross-talk rates for finite bath occupancies.

show abstract

Zero-phonon lines of systems with different dimensions and unconventional vibronic interactions

Cited by 7 publications

References 43 publications

Molecule-photon interactions in phononic environments

Molecule-photon interactions in phononic environments

Room Temperature Optical Thermometry Based on the Luminescence of the SiV Defects in Diamond

Molecule-photon interactions in phononic environments

Contact Info

Product

Resources

About