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Total Size:
10.3 MB
Info Hash:
792FB308CA9016FEB2514549A1889B8CEF12C7A6
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Added:
Oct. 9, 2025, 2:03 p.m.
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(Last updated: Oct. 9, 2025, 2:04 p.m.)
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| Reitz M. Quantum Optics with Molecules 2022.pdf | 10.3 MB |
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SOURCE: Reitz M. Quantum Optics with Molecules 2022
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COVER
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MEDIAINFO
Textbook in PDF format Molecules constitute compact hybrid quantum optical systems that can efficiently interface mechanical degrees of freedom with optical or infrared transitions. However, the coupling of molecules to the environment typically limits their coherence times which hampers their wider use in quantum optical applications. The aim of this thesis is to understand the properties of light-coupled molecules interacting with their environment and with each other and to investigate platforms where molecular degrees of freedom can be harnessed and collective effects can be observed. To this end, for the description of molecules interacting with light, we develop an open system approach based on quantum Langevin equations. The method considers the time evolution of a polaron operator, i.e., a vibrationally-dressed electronic dipole operator and can account for all coherent and incoherent interactions. In a first step, we apply the method to Floquet engineering of infraredactive molecules and show how one can make use of strong driving of molecular vibrations to control the amplitude and coherence of vibronic sidebands. In a next step, we investigate molecules encased in crystalline host environments and coupled to optical cavities and illustrate how the coupling to the phonons of the host matrix imprints itself onto the molecular absorption and the transmission spectrum of the cavity. We also discuss the vibrationally-induced cross-talk between upper and lower polaritonic states and derive rate equations for the population transfer. We then move on to regularly spaced ensembles of dipole-dipole coupled molecules, especially in ring configurations, and discuss how the vibronic coupling affects the dispersion relation and cooperative radiative properties of the ring. In particular, by moving to a collective basis, we show molecular vibrations can be used to address collective subradiant states of the ensemble. Finally, for mesoscopic disordered ensembles of molecules strongly coupled to optical cavites, we quantitatively describe the loss mechanism from polaritonic states into the dark state manifold, providing an analytical scaling of the vacuum Rabi splitting on frequency disorder
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