We demonstrate how optical cavities can be exploited to control both valence- and core-excitations in a prototypical model transition metal complex, ferricyanide ([Fe( iii )(CN) 6 ] 3− ), in an aqueous environment. The spectroscopic signatures of hybrid light-matter polariton states are revealed in UV/Vis and X-ray absorption, and stimulated X-ray Raman signals. In an UV/Vis cavity, the absorption spectrum exhibits the single-polariton states arising from the cavity photon mode coupling to both resonant and off-resonant valence-excited states. We further show that nonlinear stimulated X-ray Raman signals can selectively probe the bipolariton states via cavity-modified Fe core-excited states. This unveils the correlation between valence polaritons and dressed core-excitations. In an X-ray cavity, core-polaritons are generated and their correlations with the bare valence-excitations appear in the linear and nonlinear X-ray spectra.
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Resonantly enhanced polariton wave mixing and parametric instability in a Floquet medium
We introduce a new theoretical approach for analyzing pump and probe experiments in non-linear systems of optical phonons. In our approach, the effect of coherently pumped polaritons is modeled as providing time-periodic modulation of the system parameters. Within this framework, propagation of the probe pulse is described by the Floquet version of Maxwell’s equations and leads to phenomena such as frequency mixing and resonant parametric production of polariton pairs. We analyze light reflection from a slab of insulating material with a strongly excited phonon-polariton mode and obtain analytic expressions for the frequency-dependent reflection coefficient for the probe pulse. Our results are in agreement with recent experiments by Cartella et al. [Proc. Natl. Acad. Sci. U. S. A. 115, 12148 (2018)], which demonstrated light amplification in a resonantly excited SiC insulator. We show that, beyond a critical pumping strength, such systems should exhibit Floquet parametric instability, which corresponds to resonant scattering of pump polaritons into pairs of finite momentum polaritons. We find that the parametric instability should be achievable in SiC using current experimental techniques and discuss its signatures, including the non-analytic frequency dependence of the reflection coefficient and the probe pulse afterglow. We discuss possible applications of the parametric instability phenomenon and suggest that similar types of instabilities can be present in other photoexcited non-linear systems.
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- Award ID(s):
- 2012023
- NSF-PAR ID:
- 10360521
- Date Published:
- Journal Name:
- The Journal of Chemical Physics
- Volume:
- 156
- Issue:
- 17
- ISSN:
- 0021-9606
- Page Range / eLocation ID:
- 174110
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Polaritons—confined light–matter waves—in van der Waals (vdW) materials are a research frontier in light–matter interactions with demonstrated advances in nanophotonics. Reflection, as a fundamental phenomenon involving waves, is particularly important for vdW polaritons, predominantly because it enables the investigation of polariton standing waves using the scanning probe technique. While previous works demonstrate a rigid phase ≈π/4 for the polariton reflection, herein is reported the altering of the polariton reflection phase by varying the geometry of polaritonic microstructures for the case study of hyperbolic surface polaritons (HSPs) in hexagonal boron nitride (hBN). Specifically, it is demonstrated that the polariton reflection phase can be systematically altered by varying the corner angle of the hBN microstructures, and that it experiences a π jump around a specific angle. This behavior, which is a consequence of the mathematical nature of the reflection coefficient, is therefore expected in other physical phenomena.
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Abstract The coupling between superconductors and oscillation cycles of light pulses, i.e., lightwave engineering, is an emerging control concept for superconducting quantum electronics. Although progress has been made towards terahertz-driven superconductivity and supercurrents, the interactions able to drive non-equilibrium pairing are still poorly understood, partially due to the lack of measurements of high-order correlation functions. In particular, the sensing of exotic collective modes that would uniquely characterize light-driven superconducting coherence, in a way analogous to the Meissner effect, is very challenging but much needed. Here we report the discovery of parametrically driven superconductivity by light-induced order-parameter collective oscillations in iron-based superconductors. The time-periodic relative phase dynamics between the coupled electron and hole bands drives the transition to a distinct parametric superconducting state out-of-equalibrium. This light-induced emergent coherence is characterized by a unique phase–amplitude collective mode with Floquet-like sidebands at twice the Higgs frequency. We measure non-perturbative, high-order correlations of this parametrically driven superconductivity by separating the terahertz-frequency multidimensional coherent spectra into pump–probe, Higgs mode and bi-Higgs frequency sideband peaks. We find that the higher-order bi-Higgs sidebands dominate above the critical field, which indicates the breakdown of susceptibility perturbative expansion in this parametric quantum matter.more » « less
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Abstract Several investigators have taken advantage of electromagnetic shunt-tuned mass dampers to achieve concurrent vibration mitigation and energy harvesting. For nonlinear structures such as the Duffing oscillator, it has been shown that the novel nonlinear electromagnetic resonant shunt-tuned mass damper inerter (NERS-TMDI) can mitigate vibration and extract energy for a wider range of frequencies and forcing amplitudes when compared to competing technologies. However, nonlinear systems such as the NERS-TMDI are known to exhibit complex stability behavior, which can strongly influence their performance in simultaneous vibration control and energy harvesting. To address this problem, this paper conducts a global stability analysis of the novel NERS-TMDI using three approaches: the multi-parametric recursive continuationWe emphasize that these assume method, Floquet theory, and Lyapunov exponents. A comprehensive parametric analysis is also performed to evaluate the impact of key design parameters on the global stability of the system. The outcome indicates the existence of complex nonlinear behavior, such as detached resonance curves, and the transition of periodic stable solutions to chaotic solutions. Additionally, a parametric study demonstrates that the nonlinear stiffness has a minimal impact on the linear stability of the system but can significantly impact the nonlinear stability performance, while the transducer coefficient has an impact on the linear and nonlinear stability NERS-TMDI. Finally, the global sensitivity analysis is performed relative to system parameters to quantify the impact of uncertainty in system parameters on the dynamics. Overall, our findings show that simultaneous vibration control and energy harvesting come with a considerable instability trade-off that limits the range of operation of the NERS-TMDI.
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- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1063/5.0091718
