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arXiv:1511.00399

The effect of permanent dipole moment on the polar molecule cavity quantum electrodynamics

Jingyun Zhao, Li‐Guo Qin, Xunming Cai, Qiang Lin, Zhongyang Wang

Published Nov 2, 2015• 0 citations
arXivHTMLPDF

Abstract

A dressed-state perturbation theory beyond the rotating waveapproxi-mation (RWA) is presented to investigate the interaction between a two level electronic transition of the polar molecules and a quantized cavity field. Analytical expressions can be explicitly derived for both the ground- and excited-state-energy spectrums and wave functions of the system, where the contribution of permanent dipole moments (PDM) and the counter-rotating wave term (CRT) can be shown separately. The validity of these explicit results is discussed by comparing with the direct numerical simulation. Comparing to CRT coupling, PDM results in the coupling of more dressed states and the energy shift proportional to the square of the normalized permanent dipole difference, and a greater Bloch-Siegert shift could be produced in giant dipole molecule cavity QED. In addition, our method could also be extended to the solution of two-level atom Rabi model Hamiltonian beyond the RWA.

DOI
10.48550/arxiv.1511.00399

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A dressed-state perturbation theory beyond the rotating waveapproxi-mation (RWA) is presented to investigate the interaction between a two level electronic transition of the polar molecules and a quantized cavity field. Analytical expressions can be explicitly derived for both the ground- and excited-state-energy spectrums and wave functions of the system, where the contribution of permanent dipole moments (PDM) and the counter-rotating wave term (CRT) can be shown separately. The validity of these explicit results is discussed by comparing with the direct numerical simulation. Comparing to CRT coupling, PDM results in the coupling of more dressed states and the energy shift proportional to the square of the normalized permanent dipole difference, and a greater Bloch-Siegert shift could be produced in giant dipole molecule cavity QED. In addition, our method could also be extended to the solution of two-level atom Rabi model Hamiltonian beyond the RWA.
A dressed-state perturbation theory beyond the rotating wave approximation (RWA) is presented to investigate the interaction between a two level electronic transition of the polar molecules and a quantized cavity field.Analytical expressions can be explicitly derived for both the ground-and excited-state-energy spectrums and wave functions of the system, where the contribution of permanent dipole moments (PDM) and the counter-rotating wave term (CRT) can be shown separately.The validity of these explicit results is discussed by comparing with the direct numerical simulation.Comparing to CRT coupling, PDM results in the coupling of more dressed states and the energy shift proportional to the square of the normalized permanent dipole difference, and a greater Bloch-Siegert shift could be produced in giant dipole molecule cavity QED.In addition, our method could also be extended to the solution of two-level atom Rabi model Hamiltonian beyond the RWA.
A dressed-state perturbation theory beyond the rotating wave approximation(RWA) is presented to investigate the interaction between a two-level electronic transition of polar molecules and a quantized cavity field. Analytical expressions can be explicitly derived for both the ground- and excited-state-energy spectrums and wave functions of the system, where the contribution of permanent dipole moments(PDM) and the counter-rotating wave term(CRT) can be shown separately.The validity of these explicit results is discussed by comparison with the direct numerical simulation. Compared to the CRT coupling, PDM results in the coupling of more dressed states and the energy shift is proportional to the square of the normalized permanent dipole difference, and a greater Bloch–Siegert shift can be produced in the giant dipole molecule cavity QED. In addition, our method can also be extended to the solution of the two-level atom Rabi model Hamiltonian beyond the RWA.更多还原
We investigate the transitions between energy levels and parity symmetry in an effective two-level polar molecule system strongly coupled with a quantized harmonic oscillator. By the dressed-state perturbation theory, the transition diagrams between the dressed-state energy levels are presented clearly and show that the odd (even) parity symmetry is broken by the permanent dipole moment (PDM) of the polar molecules. By the analytical and numerical methods, we find that when the coupling strength and the PDM increase, the more frequency components are induced by the counter-rotating terms and PDM.
The Rabi Hamiltonian, describing the interaction between a two-level atomic system and a single-cavity mode of the electromagnetic field, is one of the fundamental models in quantum optics. The model becomes exactly solvable by considering an atom without permanent dipole moments, whose excitation energy is quasiresonant with the cavity photon energy, and by neglecting the nonresonant (counter-rotating) terms. In this case, after including the decay of either the atom or the cavity mode to a continuum, one can derive the well-known phenomenology of quasiresonant transitions, including the fluorescence triplets. In this work we consider the most general Rabi model, incorporating the effects of permanent atomic electric dipole moments. Based on a perturbative analysis, we compare the intensities of emission lines induced by rotating terms, counter-rotating terms, and parity-symmetry-breaking terms in order to identify the parameter regimes in which these different contributions play a significant role. The analysis reveals that the emission strength related to the existence of permanent dipoles may surpass the one due to the counter-rotating interaction terms but is usually much weaker than the emission due to the main, resonant coupling. This ratio can be modified in systems with a reduced dimensionality or by engineering the energy spectral density of the continuum.
Abstract The spectrum and energy dynamics for a system that comprises a molecule interacting with a cavity photon is analyzed, taking into account the effect of both molecular vibrations and counter‐rotating terms (CR) in the dipole Hamiltonian. The CR terms do not have a strong effect on the spectrum even for moderately large values of the exciton‐photon interaction. However, it is shown that the polariton subspace is governed by an effective Quantum‐Rabi Hamiltonian, where polaritons act as a two‐level system and the phonons play the role of cavity photons. The effect of the CR terms is amplified in the dynamics: as the vibrations reduce the effective photon‐exciton coupling, small Bloch‐Siegert energy shifts can bring the system out of resonance.
Molecular polaritons within the mid-infrared regime have emerged as a source for modifying and manipulating molecular and photonic properties. However, the development of new methodologies for photon generation is still a challenge in nanophotonics. We propose a molecular model based on the Holstein-quantum-Rabi Hamiltonian, which also incorporates realistic dipole moments and nonadiabatic couplings among electronic excited states, to study the ultrafast photodynamics of diatomic molecules in confined electromagnetic fields within quantized cavities. In addition to vibronic transitions due to intrinsic nonadiabatic couplings, two types of light-induced crossings emerge: one type is located at molecular nuclear geometries where the rotating wave approximation is fulfilled, and another type appears at different geometries where counter-rotating transitions may occur. We make a comprehensive study of polariton photodynamics within a time window of a few tens of femtoseconds, where dissipative mechanisms do not influence the polariton photodynamics. We stress the dramatic change of the polariton energy spectrum as a function of the Huang-Rhys factor when nonadiabatic couplings are included in the model. We conclude that both the molecular nonadiabatic couplings and, more specifically, the counter-rotating couplings in the cavity-molecule interaction play a crucial role in converting vibronic energy into photons through excited dressed states. We also show that the sign of the Huang-Rhys factor has a significant impact on this photon conversion. Our work paves the way for the development of many-photon generation powered by strong light-matter interaction, along with potential applications using alkaline earth monohydride molecules.