- Award ID(s):
- Publication Date:
- NSF-PAR ID:
- Journal Name:
- Chemical Science
- Page Range or eLocation-ID:
- 1290 to 1298
- Sponsoring Org:
- National Science Foundation
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We investigate the Polariton induced conical intersection (PICI) created from coupling a diatomic molecule with the quantized photon mode inside an optical cavity, and the corresponding Berry Phase effects. We use the rigorous Pauli–Fierz Hamiltonian to describe the quantum light-matter interactions between a LiF molecule and the cavity, and use the exact quantum propagation to investigate the polariton quantum dynamics. The molecular rotations relative to the cavity polarization direction play a role as the tuning mode of the PICI, resulting in an effective CI even within a diatomic molecule. To clearly demonstrate the dynamical effects of the Berry phase, we construct two additional models that have the same Born–Oppenheimer surface, but the effects of the geometric phase are removed. We find that when the initial wavefunction is placed in the lower polaritonic surface, the Berry phase causes a π phase-shift in the wavefunction after the encirclement around the CI, indicated from the nuclear probability distribution. On the other hand, when the initial wavefunction is placed in the upper polaritonic surface, the geometric phase significantly influences the couplings between polaritonic states and therefore, the population dynamics between them. These BP effects are further demonstrated through the photo-fragment angular distribution. PICI createdmore »
Polariton relaxation under vibrational strong coupling: Comparing cavity molecular dynamics simulations against Fermi’s golden rule rateUnder vibrational strong coupling (VSC), the formation of molecular polaritons may significantly modify the photo-induced or thermal properties of molecules. In an effort to understand these intriguing modifications, both experimental and theoretical studies have focused on the ultrafast dynamics of vibrational polaritons. Here, following our recent work [Li et al., J. Chem. Phys. 154, 094124 (2021)], we systematically study the mechanism of polariton relaxation for liquid CO 2 under a weak external pumping. Classical cavity molecular dynamics (CavMD) simulations confirm that polariton relaxation results from the combined effects of (i) cavity loss through the photonic component and (ii) dephasing of the bright-mode component to vibrational dark modes as mediated by intermolecular interactions. The latter polaritonic dephasing rate is proportional to the product of the weight of the bright mode in the polariton wave function and the spectral overlap between the polariton and dark modes. Both these factors are sensitive to parameters such as the Rabi splitting and cavity mode detuning. Compared to a Fermi’s golden rule calculation based on a tight-binding harmonic model, CavMD yields a similar parameter dependence for the upper polariton relaxation lifetime but sometimes a modest disagreement for the lower polariton. We suggest that this disagreement resultsmore »
Abstract Engineering the properties of quantum materials via strong light-matter coupling is a compelling research direction with a multiplicity of modern applications. Those range from modifying charge transport in organic molecules, steering particle correlation and interactions, and even controlling chemical reactions. Here, we study the modification of the material properties via strong coupling and demonstrate an effective inversion of the excitonic band-ordering in a monolayer of WSe 2 with spin-forbidden, optically dark ground state. In our experiments, we harness the strong light-matter coupling between cavity photon and the high energy, spin-allowed bright exciton, and thus creating two bright polaritonic modes in the optical bandgap with the lower polariton mode pushed below the WSe 2 dark state. We demonstrate that in this regime the commonly observed luminescence quenching stemming from the fast relaxation to the dark ground state is prevented, which results in the brightening of this intrinsically dark material. We probe this effective brightening by temperature-dependent photoluminescence, and we find an excellent agreement with a theoretical model accounting for the inversion of the band ordering and phonon-assisted polariton relaxation.
Modulation-based control and locking of lasers, filters and other photonic components is a ubiquitous function across many applications that span the visible to infrared (IR), including atomic, molecular and optical (AMO), quantum sciences, fiber communications, metrology, and microwave photonics. Today, modulators used to realize these control functions consist of high-power bulk-optic components for tuning, sideband modulation, and phase and frequency shifting, while providing low optical insertion loss and operation from DC to 10s of MHz. In order to reduce the size, weight and cost of these applications and improve their scalability and reliability, modulation control functions need to be implemented in a low loss, wafer-scale CMOS-compatible photonic integration platform. The silicon nitride integration platform has been successful at realizing extremely low waveguide losses across the visible to infrared and components including high performance lasers, filters, resonators, stabilization cavities, and optical frequency combs. Yet, progress towards implementing low loss, low power modulators in the silicon nitride platform, while maintaining wafer-scale process compatibility has been limited. Here we report a significant advance in integration of a piezo-electric (PZT, lead zirconate titanate) actuated micro-ring modulation in a fully-planar, wafer-scale silicon nitride platform, that maintains low optical loss (0.03 dB/cm in a 625 µmmore »
We show that concept of parity-time (PT) symmetry can be expanded to include mixed photon-exciton modes by demonstrating that eigenmodes of active (pumped) strongly coupled cavity polaritons with population inversion exhibit characteristics that are remarkably akin to those of coupled photonic structures with parity-time symmetry. The exceptional point occurs when the Rabi splitting of polariton branches inherent in passive polaritonic systems decreases with increase in pumping, leading to population inversion, and eventually two polaritonic modes merge into a single mode, thus manifesting the frequency pulling effect inherent to all lasers. But, remarkably, this exceptional point occurs below the lasing threshold. Furthermore, unlike most manifestations of PT symmetry in optics, which are observed in the interaction between two analogous photonic modes in waveguides or cavities, in this work the exceptional point is found in interaction between two very dissimilar modes—one photonic and one material excitation (exciton). Aside from fundamentally noteworthy expansion of the concept of PT symmetry to new systems, there is a prospect of using the exceptional point in polaritons for practical applications, such as sensing.