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Register a new userFreezing molecules with light: How long can one maintain a non-equilibrium molecular geometry by strong light-matter coupling?
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In molecular photochemistry, the non-equilibrium character and subsequent ultrafast relaxation dynamics of photoexcitations near the Franck-Condon region limit the control of their chemical reactivity. We address how to harness strong light-matter coupling in optical microcavities to isolate and preferentially select specific reaction pathways out of the myriad of possibilities present in large-scale complex systems. Using Fermis Golden Rule and realistic molecular parameters, we estimate the extent to which molecular configurations can be locked into non-equilibrium excited state configurations for timescales well beyond their natural relaxation times. For upper polaritons--which are largely excitonic in character, molecular systems can be locked into their ground state geometries for tens to thousands of picoseconds and varies with the strength of the exciton/phonon coupling (Huang-Rhys parameter). On the other hand, relaxed LP lifetimes are nearly uniformly distributed between 2.1-2.4,ps and are nearly independent of the Huang-Rhys parameter.
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The optical properties of transition metal dichalcogenide monolayers are widely dominated by excitons, Coulomb-bound electron-hole pairs. These quasi-particles exhibit giant oscillator strength and give rise to narrow-band, well-pronounced optical transitions, which can be brought into resonance with electromagnetic fields in microcavities and plasmonic nanostructures. Due to the atomic thinness and robustness of the monolayers, their integration in van der Waals heterostructures provides unique opportunities for engineering strong light-matter coupling. We review first results in this emerging field and outline future opportunities and challenges.
Optical detection and spectroscopy of single molecules has become an indispensable tool in biological imaging and sensing. Its success is based on fluorescence of organic dye molecules under carefully engineered laser illumination. In this paper we demonstrate optical detection of single molecules on a wide-field microscope with an illumination based on a commercially available, green light-emitting diode. The results are directly compared with laser illumination in the same experimental configuration. The setup and the limiting factors, such as light transfer to the sample, spectral filtering and the resulting signal-to-noise ratio are discussed. A theoretical and an experimental approach to estimate these parameters are presented. The results can be adapted to other single emitter and illumination schemes.
The propagation of $N$ photons in one dimensional waveguides coupled to $M$ qubits is discussed, both in the strong and ultrastrong qubit-waveguide coupling. Special emphasis is placed on the characterisation of the nonlinear response and its linear limit for the scattered photons as a function of $N$, $M$, qubit inter distance and light-matter coupling. The quantum evolution is numerically solved via the Matrix Product States technique. Both the time evolution for the field and qubits is computed. The nonlinear character (as a function of $N/M$) depends on the computed observable. While perfect reflection is obtained for $N/M cong 1$, photon-photon correlations are still resolved for ratios $N/M= 2/20$. Inter-qubit distance enhances the nonlinear response. Moving to the ultrastrong coupling regime, we observe that inelastic processes are emph{robust} against the number of qubits and that the qubit-qubit interaction mediated by the photons is qualitatively modified. The theory developed in this work modelises experiments in circuit QED, photonic crystals and dielectric waveguides.
Polariton-based devices require materials where light-matter coupling under ambient conditions exceeds losses, but our current selection of such materials is limited. Here we measured the dispersion of polaritons formed by the $A$ and $B$ excitons in thin MoS$_2$ slabs by imaging their optical near fields. We combined fully tunable laser excitation in the visible with a scattering near-field optical microscope to excite polaritons and image their optical near fields. We obtained the properties of bulk MoS$_2$ from fits to the slab dispersion. The in-plane excitons are in the strong regime of light-matter coupling with a coupling strength ($40-100,$meV) that exceeds their losses by at least a factor of two. The coupling becomes comparable to the exciton binding energy, which is known as very strong coupling. MoS$_2$ and other transition metal dichalcogenides are excellent materials for future polariton devices.
Quantum geometry has been identified as an important ingredient for the physics of quantum materials and especially of flat-band systems, such as moire materials. On the other hand, the coupling between light and matter is of key importance across disciplines and especially for Floquet and cavity engineering of solids. Here we present fundamental relations between light-matter coupling and quantum geometry of Bloch wave functions, with a particular focus on flat-band and moire materials, in which the quenching of the electronic kinetic energy could allow one to reach the limit of strong light-matter coupling more easily than in highly dispersive systems. We show that, despite the fact that flat bands have vanishing band velocities and curvatures, light couples to them via geometric contributions. Specifically, the intra-band quantum metric allows diamagnetic coupling inside a flat band; the inter-band Berry connection governs dipole matrix elements between flat and dispersive bands. We illustrate these effects in two representative model systems: (i) a sawtooth quantum chain with a single flat band, and (ii) a tight-binding model for twisted bilayer graphene. For (i) we highlight the importance of quantum geometry by demonstrating a nonvanishing diamagnetic light-matter coupling inside the flat band. For (ii) we explore the twist-angle dependence of various light-matter coupling matrix elements. Furthermore, at the magic angle corresponding to almost flat bands, we show a Floquet-topological gap opening under irradiation with circularly polarized light despite the nearly vanishing Fermi velocity. We discuss how these findings provide fundamental design principles and tools for light-matter-coupling-based control of emergent electronic properties in flat-band and moire materials.
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