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Applied Sciences

Fluorimetry in the Strong-Coupling Regime: From a Fundamental Perspective to Engineering New Tools for Tracing and Marking Materials and Objects

Mohamed Hatifi, Dimitrije Mara, Bojana M. Bokić, Rik Van Deun, Brian Stout, Emmanuel Lassalle, Branko Kolarić, Thomas Durt

Published Sep 15, 2022• 1 citation
Publisher

Abstract

Under exceptional circumstances, light and molecules bond together, creating new hybrid light–matter states with far-reaching consequences for these strongly coupled entities. The present article describes the quantum-mechanical foundation of strong-coupling and experimental evidence for molding the radiation properties of nanoprobes by strong-coupling. When applied to tracing and marking, the new fluorometry technique proposed here, which harnesses strong-coupling, has a triple advantage compared to its classical counterparts such as DNA tracing. It is fast, and its signal-to-noise ratio can be improved by spectral filtering; moreover, it reveals a specific quantum signature of the strong-coupling, which is extremely difficult to reproduce classically, thereby opening the door to new anti-counterfeiting strategies.

DOI
10.3390/app12189238

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Under exceptional circumstances, light and molecules bond together, creating new hybrid light–matter states with far-reaching consequences for these strongly coupled entities. The present article describes the quantum-mechanical foundation of strong-coupling and experimental evidence for molding the radiation properties of nanoprobes by strong-coupling. When applied to tracing and marking, the new fluorometry technique proposed here, which harnesses strong-coupling, has a triple advantage compared to its classical counterparts such as DNA tracing. It is fast, and its signal-to-noise ratio can be improved by spectral filtering; moreover, it reveals a specific quantum signature of the strong-coupling, which is extremely difficult to reproduce classically, thereby opening the door to new anti-counterfeiting strategies.
Abstract When atoms come together and bond, these new states are called molecules and their properties determine many aspects of our daily life. Strangely enough, it is conceivable for light and molecules to bond, creating new hybrid light–matter states with far‐reaching consequences for these strongly coupled materials. Even stranger, there is no “real” light needed to obtain the effects; it simply appears from the vacuum, creating “something from nothing.” Surprisingly, the setup required to create these materials has become moderately straightforward. In its simplest form, one only needs to put a strongly absorbing material at the appropriate place between two mirrors, and quantum magic can appear. Only recently has it been discovered that strong coupling can affect a host of significant effects at a material and molecular level, which were thought to be independent of the “light” environment: phase transitions, conductivity, chemical reactions, etc. This review addresses the fundamentals of this opportunity: the quantum mechanical foundations, the relevant plasmonic and photonic structures, and a description of the various applications, connecting material chemistry with quantum information, entanglement, nonlinear optics, and chemical reactivity. Ultimately, revealing the interplay between light and matter in this new regime opens attractive avenues for various new technologies.
Resonance interaction between a molecular transition and a confined electromagnetic field can reach the coupling regime where coherent exchange of energy between light and matter becomes reversible. In this case, two new hybrid states separated in energy are formed instead of independent eigenstates, which is known as Rabi splitting. This modification of the energy spectra of the system offers new possibilities for controlled impact on various fundamental properties of coupled matter (such as the rate of chemical reactions and the conductivity of organic semiconductors). To date, the strong coupling regime has been demonstrated in many configurations under different ambient conditions. However, there is still no comprehensive approach to determining parameters for achieving the strong coupling regime for a wide range of practical applications. In this review, a detailed analysis of various systems and corresponding conditions for reaching strong coupling is carried out and their advantages and disadvantages, as well as the prospects for application, are considered. The review also summarizes recent experiments in which the strong coupling regime has led to new interesting results, such as the possibility of collective strong coupling between X-rays and matter excitation in a periodic array of Fe isotopes, which extends the applications of quantum optics; a strong amplification of the Raman scattering signal from a coupled system, which can be used in surface-enhanced and tip-enhanced Raman spectroscopy; and more efficient second-harmonic generation from the low polaritonic state, which is promising for nonlinear optics. The results reviewed demonstrate great potential for further practical applications of strong coupling in the fields of photonics (low-threshold lasers), quantum communications (switches), and biophysics (molecular fingerprinting).
The strong coupling regime of photons and quantum materials inside optical cavities has emerged as a promising environment for manipulating states of matter with light. Here, in turn, we show that photons bear witness to cavity quantum-electrodynamical modifications of the material, leading to profoundly non-classical properties of light passing through the cavity. By generalizing quantum-optical input-output relations to correlated quantum materials, we study the second-order photon coherence g2(t) and demonstrate that antibunching of transmitted photons serves as direct evidence of light-induced changes to the cavity-embedded material. We show that materials near a quantum critical point can realize a collective many-body photon blockade, enabling the generation of single photons or Einstein-Podolsky-Rosen pairs via leveraging strong matter fluctuations. Our findings provide new routes for interrogating and harnessing cavity-embedded quantum materials as quantum light sources, as a resource for photon-based computation and quantum sensing.
Molecular complexes are held together via a variety of bonds, but they all share the common feature that their individual entities are in contact. In this work, we introduce and demonstrate the concept of a \textit{molecular optical bond}, resulting from the far-field electromagnetic coupling of several molecules via a shared mode of an optical microcavity. We discuss a collective enhancement of the vacuum Rabi splitting and study super- and sub-radiant states that arise from the cavity-mediated coupling both in the resonant and dispersive regimes. Moreover, we demonstrate a two-photon transition that emerges between the ground and excited states of the new optical compound. Our experimental data are in excellent agreement with the predictions of the Tavis-Cummings Hamiltonian and open the door to the realization of hybrid light-matter materials.
Spectral measurements provide fundamental insights into wave systems by revealing resonances, mode hybridization, and light-matter interactions. However, intrinsic dissipation and measurement-related spectral broadening often obscure the spectral signatures of the underlying hybridized light-matter states. Here, we establish a temporal Fourier optics framework based on a space-time Fourier correspondence, which interprets spectral broadening as the Fourier counterpart of temporal attenuation. This perspective introduces a temporal point-spread function (TPSF) that enables direct, synthesis-free reconstruction of the underlying spectral response from experimentally measured spectra by compensating for effective temporal decay before transformation back to the frequency domain. We experimentally validate the framework using deterministic single-molecule Au nanosphere dimers and open Au@Ag nanorod- and nanotriangle-based plasmonic nanocavities coupled to J-aggregate excitons. Across these distinct platforms, TPSF consistently resolves hidden upper and lower polaritonic branches, revealing hybridized light-matter states and strong coupling that remain inaccessible in conventional scattering spectra. The reconstructed spectra agree closely with the recently developed complex-frequency formalism while providing a substantially simpler and experimentally accessible implementation. More broadly, temporal Fourier optics establishes a general framework for recovering dissipation-obscured spectral information, opening new opportunities for spectroscopy, imaging, sensing, and inverse wave measurements across photonics and wave physics.