Light-matter Coupling Strength Research Articles

Magnon dispersion, magnetization, and thermodynamic properties of 2D-Sc/GaAs diluted magnetic semiconductor (DMS)

In this paper, the effect of magnon scattering, light–matter coupling strength, temperature, and applied dc field H0 on magnon dispersion, density of magnons, magnetization, and thermodynamic properties of 2D-Sc/GaAs DMS material is studied. The Green function formalism is used to find the magnon dispersion and density in single-mode excitation employing the quantum field theory. Our findings indicate that ferromagnetic phase change is obtained within a limited low-temperature range based on the product Ω0T5/2, which remains below unity and varies with the amount of magnon scattering factor Ω0. It was presumed that the density of localized magnetic impurities can be controlled by taking into account the numerical stability with the number of holes required for mediation, and therefore, a scandium (Sc) dopant and its kind, which have a double functionality of creating holes and adding magnetic impurities from their 3d suborbital, are the best choice to replace those with higher spin magnetic moments. We also observe that the magnetic curves broaden as the temperature further rises and decrease with the enhancement of the magnon scattering factor, perhaps, due to quenching of fermionic spins ceasing the interband excitation. However, in the absence of this factor, the magnetization decreases linearly with the increase in the temperature, breaking the Bloch T3/2 low, perhaps, introducing anomalous condition to such 2D materials. The light–matter coupling strength and the dc field H0 are alleged to be responsible for the formation of the energy gap and variation of magnon dispersion. This work suggests that there is a point above which the temperature TC may not rise with the increase in the impurity concentration x due to magnon scattering, distressing the entire thermodynamic property.

Resonance Enhancement of Vibrational Polariton Chemistry Obtained from the Mixed Quantum-Classical Dynamics Simulations.

We applied a variety of mixed quantum-classical (MQC) approaches to simulate the VSC-influenced reaction rate constant. All of these MQC simulations treat the key vibrational levels associated with the reaction coordinate in the quantum subsystem (as quantum states), whereas all other degrees of freedom (DOFs) are treated inside the classical subsystem. We find that, as long as we have the quantum state descriptions for the vibrational DOFs, one can correctly describe the VSC resonance condition when the cavity frequency matches the bond vibrational frequency. This correct resonance behavior can be obtained regardless of the detailed MQC methods that one uses. The results suggest that the MQC approaches can generate semiquantitative agreement with the exact results for rate constant changes when changing the cavity frequency, the light-matter coupling strength, or the cavity lifetime. The finding of this work suggests that one can use computationally economic MQC approaches to explore the collective coupling scenario when many molecules are collectively coupled to many cavity modes in the future.

Molecular van der Waals Fluids in Cavity Quantum Electrodynamics.

Intermolecular van der Waals interactions are central to chemical and physical phenomena ranging from biomolecule binding to soft-matter phase transitions. In this work, we demonstrate that strong light-matter coupling can be used to control the thermodynamic properties of many-molecule systems. Our analyses reveal orientation dependent single molecule energies and interaction energies for van der Waals molecules. For example, we find intermolecular interactions that depend on the distance between the molecules R as R-3 and R0. Moreover, we employ ab initio cavity quantum electrodynamics calculations to develop machine-learning-based interaction potentials for molecules inside optical cavities. By simulating systems ranging from 12 H2 to 144 H2 molecules, we observe varying degrees of orientational order because of cavity-modified interactions, and we explain how quantum nuclear effects, light-matter coupling strengths, number of cavity modes, molecular anisotropies, and system size all impact the extent of orientational order.

Engineered planar plasmonic reflector for polaritonic mode confinement [Invited

It was recently demonstrated that, in deep subwavelength gap resonators coupled to two-dimensional electron gases, propagating plasmons can lead to energy leakage and prevent the formation of polaritonic resonances. This process, akin to Landau damping, limits the achievable field confinement and thus the value of light-matter coupling strength. In this work, we show how plasmonic reflectors can be used to create an artificial energy stopband in the plasmon dispersion, confining them and enabling the recovery of the polaritonic resonances. Using this approach we demonstrate a normalized light-matter coupling ratio of Ω R ω0=0.36 employing a single doped quantum well with a resonator’s gap size of 250 nm equivalent to λ/3000 in vacuum, a geometry in which the polaritonic resonances would not be observable in the absence of the plasmonic reflectors.

Quantum dynamics simulations of the 2D spectroscopy for exciton polaritons.

We develop an accurate and numerically efficient non-adiabatic path-integral approach to simulate the non-linear spectroscopy of exciton-polariton systems. This approach is based on the partial linearized density matrix approach to model the exciton dynamics with explicit propagation of the phonon bath environment, combined with a stochastic Lindblad dynamics approach to model the cavity loss dynamics. Through simulating both linear and polariton two-dimensional electronic spectra, we systematically investigate how light-matter coupling strength and cavity loss rate influence the optical response signal. Our results confirm the polaron decoupling effect, which is the reduced exciton-phonon coupling among polariton states due to the strong light-matter interactions. We further demonstrate that the polariton coherence time can be significantly prolonged compared to the electronic coherence outside the cavity.

Resonance theory and quantum dynamics simulations of vibrational polariton chemistry.

We present numerically exact quantum dynamics simulations using the hierarchical equation of motion approach to investigate the resonance enhancement of chemical reactions due to the vibrational strong coupling (VSC) in polariton chemistry. The results reveal that the cavity mode acts like a "rate-promoting vibrational mode" that enhances the ground state chemical reaction rate constant when the cavity mode frequency matches the vibrational transition frequency. The exact simulation predicts that the VSC-modified rate constant will change quadratically as the light-matter coupling strength increases. When changing the cavity lifetime from the lossy limit to the lossless limit, the numerically exact results predict that there will be a turnover of the rate constant. Based on the numerical observations, we present an analytic rate theory to explain the observed sharp resonance peak of the rate profile when tuning the cavity frequency to match the quantum transition frequency of the vibrational ground state to excited states. This rate theory further explains the origin of the broadening of the rate profile. The analytic rate theory agrees with the numerical results under the golden rule limit and the short cavity lifetime limit. To the best of our knowledge, this is the first analytic theory that is able to explain the sharp resonance behavior of the VSC-modified rate profile when coupling an adiabatic ground state chemical reaction to the cavity. We envision that both the numerical analysis and the analytic theory will offer invaluable theoretical insights into the fundamental mechanism of the VSC-induced rate constant modifications in polariton chemistry.

Upper bounds on collective light-matter coupling strength with plasmonic meta-atoms

Upper bounds on collective light-matter coupling strength with plasmonic meta-atoms

Manipulating hydrogen bond dissociation rates and mechanisms in water dimer through vibrational strong coupling

The vibrational strong coupling (VSC) between molecular vibrations and cavity photon modes has recently emerged as a promising tool for influencing chemical reactivities. Despite numerous experimental and theoretical efforts, the underlying mechanism of VSC effects remains elusive. In this study, we combine state-of-art quantum cavity vibrational self-consistent field/configuration interaction theory (cav-VSCF/VCI), quasi-classical trajectory method, along with the quantum-chemical CCSD(T)-level machine learning potential, to simulate the hydrogen bond dissociation dynamics of water dimer under VSC. We observe that manipulating the light-matter coupling strength and cavity frequencies can either inhibit or accelerate the dissociation rate. Furthermore, we discover that the cavity surprisingly modifies the vibrational dissociation channels, with a pathway involving both water fragments in their ground vibrational states becoming the major channel, which is a minor one when the water dimer is outside the cavity. We elucidate the mechanisms behind these effects by investigating the critical role of the optical cavity in modifying the intramolecular and intermolecular coupling patterns. While our work focuses on single water dimer system, it provides direct and statistically significant evidence of VSC effects on molecular reaction dynamics.

Macroscopic transition metal dichalcogenides monolayers with uniformly high optical quality

The unique optical properties of transition metal dichalcogenide (TMD) monolayers have attracted significant attention for both photonics applications and fundamental studies of low-dimensional systems. TMD monolayers of high optical quality, however, have been limited to micron-sized flakes produced by low-throughput and labour-intensive processes, whereas large-area films are often affected by surface defects and large inhomogeneity. Here we report a rapid and reliable method to synthesize macroscopic-scale TMD monolayers of uniform, high optical quality. Using 1-dodecanol encapsulation combined with gold-tape-assisted exfoliation, we obtain monolayers with lateral size > 1 mm, exhibiting exciton energy, linewidth, and quantum yield uniform over the whole area and close to those of high-quality micron-sized flakes. We tentatively associate the role of the two molecular encapsulating layers as isolating the TMD from the substrate and passivating the chalcogen vacancies, respectively. We demonstrate the utility of our encapsulated monolayers by scalable integration with an array of photonic crystal cavities, creating polariton arrays with enhanced light-matter coupling strength. This work provides a pathway to achieving high-quality two-dimensional materials over large areas, enabling research and technology development beyond individual micron-sized devices.

Ab Initio Molecular Cavity Quantum Electrodynamics Simulations Using Machine Learning Models.

We present a mixed quantum-classical simulation of polariton dynamics for molecule-cavity hybrid systems. In particular, we treat the coupled electronic-photonic degrees of freedom (DOFs) as the quantum subsystem and the nuclear DOFs as the classical subsystem and use the trajectory surface hopping approach to simulate non-adiabatic dynamics among the polariton states due to the coupled motion of nuclei. We use the accurate nuclear gradient expression derived from the Pauli-Fierz quantum electrodynamics Hamiltonian without making further approximations. The energies, gradients, and derivative couplings of the molecular systems are obtained from the on-the-fly simulations at the level of complete active space self-consistent field (CASSCF), which are used to compute the polariton energies and nuclear gradients. The derivatives of dipoles are also necessary ingredients in the polariton nuclear gradient expression but are often not readily available in electronic structure methods. To address this challenge, we use a machine learning model with the Kernel ridge regression method to construct the dipoles and further obtain their derivatives, at the same level as the CASSCF theory. The cavity loss process is modeled with the Lindblad jump superoperator on the reduced density of the electronic-photonic quantum subsystem. We investigate the azomethane molecule and its photoinduced isomerization dynamics inside the cavity. Our results show the accuracy of the machine-learned dipoles and their usage in simulating polariton dynamics. Our polariton dynamics results also demonstrate the isomerization reaction of azomethane can be effectively tuned by coupling to an optical cavity and by changing the light-matter coupling strength and the cavity loss rate.

Magnetically tuned continuous transition from weak to strong coupling in terahertz magnon polaritons

Highly tunable light-matter hybrids, magnon polaritons, have been realized in an orthoferrite crystal driven by terahertz radiation in an external magnetic field. As the magnetic field is swept, a continuous transition from weak to strong coupling via an exceptional point due to a magnetic-field-dependent light-matter coupling strength is observed.

Polaritonic Huang-Rhys Factor: Basic Concepts and Quantifying Light-Matter Interactions in Media.

The Huang-Rhys (HR) factor, a dimensionless factor that characterizes electron-phonon (vibronic) coupling, has been extensively employed to investigate a variety of material properties. In the same spirit, we propose a quantity called the polaritonic HR factor to quantitatively describe the effects of (i) light-matter coupling induced by permanent dipoles and (ii) dipole self-energy. The former leads to polaritonic displacements, while the latter is associated with the electronic coupling shift named reorganization dipole self-coupling. In the framework of macroscopic quantum electrodynamics, our theory can evaluate the polaritonic HR factor, reorganization dipole self-coupling, and modified light-matter coupling strength in an arbitrary dielectric environment without free parameters, whose magnitudes are in good agreement with the previous experimental results. We believe that this study provides a useful perspective on understanding and quantifying light-matter interactions in media.

Measuring the Magnon-Photon Coupling in Shaped Ferromagnets: Tuning of the Resonance Frequency

Cavity photons and ferromagnetic spin excitations can exchange information coherently in hybrid architectures, at speeds set by their mutual coupling strength. Speed enhancement is usually achieved by optimizing the geometry of the electromagnetic cavity. Here we show that the geometry of the ferromagnet also plays a role, by setting the fundamental frequency of the magnonic resonator. Using focused ion-beam patterning, we vary the aspect ratio of different Permalloy samples reaching operation frequencies above 10 GHz while working at low external magnetic fields. Additionally, we perform broadband ferromagnetic resonance measurements and cavity experiments that demonstrate that the light-matter coupling strength can be estimated using either open transmission lines or resonant cavities, yielding very good agreement. Finally, we describe a simple theoretical framework based on electromagnetic and micromagnetic simulations that successfully accounts for the experimental results. This approach can be used to design hybrid quantum systems exploiting magnetostatic mode excited in ferromagnets of arbitrary size and shape and to tune their operation conditions.

Versatile Tunable Microresonator for the Light-Matter Interaction Studying in the Strong-Coupling Mode

The interaction between an ensemble of molecules and an electromagnetic field in a highly limited volume makes it possible to control the properties of a substance and, therefore, is an exceptionally promising area of research. The most common way to achieve weak or strong light-matter coupling is to place an ensemble of molecules in a micron-sized resonator. In such a system,the interaction of light with matter appears in the form of a change in the spectral response of the system, which depends on the strength of the coupling between the ensemble of molecules and the modes of the resonator. Currently, there is no general and user-friendly approach that allows studying a lot of different samples in a wide optical range using the same resonator setup. The present paper describes the design of a device that makes it possible to overcome this disadvantage, speed up and facilitate the study of the light-matter interaction, and also obtain weak and strong light-matter coupling modes for a large number of samples in the UV, visible, and IR regions of the optical spectrum. The device developed here is based on the tunable unstable λ/2 Fabry-Perot microresonator, consisting of flat and convex mirrors, which satisfy the condition of plane-parallelism at least at one point of the curved mirror and can significantly reduce the mode volume. The device was used to study the effect of the strong-coupling regime on the fluorescent properties of the Rhodamine 6G (R6G) dye embedded in a boron nitride nanoparticles matrix. It was found that the use of boron nitride (h-BN) as a carrier matrix has an orienting effect on the dye molecules, that results in an increase of the light-matter coupling strength at a lower resonator mode energy required. Keywords: microspectroscopy, optical microresonator, strong coupling, boron nitride.

Универсальный перестраиваемый микрорезонатор для исследования взаимодействия света с веществом в ржиме сильной связи

The interaction between an ensemble of molecules and an electromagnetic field in a highly limited volume makes it possible to control the properties of a substance and, therefore, is an exceptionally promising area of research. The most common way to achieve weak or strong light-matter coupling is to place an ensemble of molecules in a micron-sized resonator. In such a system,the interaction of light with matter appears in the form of a change in the spectral response of the system, which depends on the strength of the coupling between the ensemble of molecules and the modes of the resonator. Currently, there is no general and user-friendly approach that allows studying a lot of different samples in a wide optical range using the same resonator setup. The present paper describes the design of a device that makes it possible to overcome this disadvantage, speed up and facilitate the study of the light-matter interaction, and also obtain weak and strong light-matter coupling modes for a large number of samples in the UV, visible, and IR regions of the optical spectrum. The device developed here is based on the tunable unstable λ/2 Fabry-Perot microresonator, consisting of flat and convex mirrors, which satisfy the condition of plane-parallelism at least at one point of the curved mirror and can significantly reduce the mode volume. The device was used to study the effect of the strong-coupling regime on the fluorescent properties of the Rhodamine 6G (R6G) dye embedded in a boron nitride nanoparticles matrix. It was found that the use of boron nitride (h-BN) as a carrier matrix has an orienting effect on the dye molecules, that results in an increase of the light-matter coupling strength at a lower resonator mode energy required.

Feedback and compensation scheme to suppress the thermal effects from a dipole trap beam for the optical fiber microcavity.

Cavity quantum electrodynamics (cavity QED) with neutral atoms is a promising platform for quantum information processing and optical fiber Fabry-Pérot microcavity with small mode volume is an important integrant for the large light-matter coupling strength. To transport cold atoms to the microcavity, a high-power optical dipole trap (ODT) beam perpendicular to the cavity axis is commonly used. However, the overlap between the ODT beam and the cavity mirrors causes thermal effects inducing a large cavity shift at the locking wavelength and a differential cavity shift at the probe wavelength which disturbs the cavity resonance. Here, we develop a feedback and compensation scheme to maintain the optical fiber microcavity resonant with the lasers at the locking and probe wavelengths simultaneously. The large cavity shift of 210 times the cavity linewidth, which makes the conventional PID scheme ineffective can be suppressed actively by a PIID feedback scheme with an additional I parameter. Differential cavity shift at the probe wavelength can be understood from the photothermal refraction and thermal expansion effects on the mirror coatings and be passively compensated by changing the frequency of the locking laser. A further normal-mode splitting measurement demonstrates the strong coupling between 85Rb atoms and cavity mode after the thermal effects are suppressed, which also confirms successful delivery and trapping of atoms into the optical cavity. This scheme can solve the thermal effects of the high-power ODT beam and will be helpful to cavity QED experimental research.

Controlling topological phases of matter with quantum light

Controlling the topological properties of quantum matter is a major goal of condensed matter physics. A major effort in this direction has been devoted to using classical light in the form of Floquet drives to manipulate and induce states with non-trivial topology. A different route can be achieved with cavity photons. Here we consider a prototypical model for topological phase transition, the one-dimensional Su-Schrieffer-Heeger model, coupled to a single mode cavity. We show that quantum light can affect the topological properties of the system, including the finite-length energy spectrum hosting edge modes and the topological phase diagram. In particular we show that depending on the lattice geometry and the strength of light-matter coupling one can either turn a trivial phase into a topological one or viceversa using quantum cavity fields. Furthermore, we compute the polariton spectrum of the coupled electron-photon system, and we note that the lower polariton branch disappears at the topological transition point. This phenomenon can be used to probe the phase transition in the Su-Schrieffer-Heeger model.

Efficient Many-Body Non-Markovian Dynamics of Organic Polaritons.

We show how to simulate a model of many molecules with both strong coupling to many vibrational modes and collective coupling to a single photon mode. We do this by combining process tensor matrix product operator methods with a mean-field approximation which reduces the dimension of the problem. We analyze the steady state of the model under incoherent pumping to determine the dependence of the polariton lasing threshold on cavity detuning, light-matter coupling strength, and environmental temperature. Moreover, by measuring two-time correlations, we study quadratic fluctuations about the mean field to calculate the photoluminescence spectrum. Our method enables one to simulate many-body systems with strong coupling to multiple environments, and to extract both static and dynamical properties.

Giant mid-IR resonant coupling to molecular vibrations in sub-nm gaps of plasmonic multilayer metafilms

Nanomaterials capable of confining light are desirable for enhancing spectroscopies such as Raman scattering, infrared absorption, and nonlinear optical processes. Plasmonic superlattices have shown the ability to host collective resonances in the mid-infrared, but require stringent fabrication processes to create well-ordered structures. Here, we demonstrate how short-range-ordered Au nanoparticle multilayers on a mirror, self-assembled by a sub-nm molecular spacer, support collective plasmon-polariton resonances in the visible and infrared, continuously tunable beyond 11 µm by simply varying the nanoparticle size and number of layers. The resulting molecule-plasmon system approaches vibrational strong coupling, and displays giant Fano dip strengths, SEIRA enhancement factors ~ 106, light-matter coupling strengths g ~ 100 cm−1, Purcell factors ~ 106, and mode volume compression factors ~ 108. The collective plasmon-polariton mode is highly robust to nanoparticle vacancy disorder and is sustained by the consistent gap size defined by the molecular spacer. Structural disorder efficiently couples light into the gaps between the multilayers and mirror, enabling Raman and infrared sensing of sub-picolitre sample volumes.

Nonperturbative waveguide quantum electrodynamics

Understanding physical properties of quantum emitters strongly interacting with quantized electromagnetic modes is one of the primary goals in the emergent field of waveguide quantum electrodynamics (QED). When the light-matter coupling strength is comparable to or even exceeds energies of elementary excitations, conventional approaches based on perturbative treatment of light-matter interactions, two-level description of matter excitations, and photon-number truncation are no longer sufficient. Here we study in and out of equilibrium properties of waveguide QED in such nonperturbative regimes on the basis of a comprehensive and rigorous theoretical approach using an asymptotic decoupling unitary transformation. We uncover several surprising features ranging from symmetry-protected many-body bound states in the continuum to strong renormalization of the effective mass and potential; the latter may explain recent experiments demonstrating cavity-induced changes in chemical reactivity as well as enhancements of ferromagnetism or superconductivity. To illustrate our general results with concrete examples, we use our formalism to study a model of coupled cavity arrays, which is relevant to experiments in superconducting qubits interacting with microwave resonators or atoms coupled to photonic crystals. We examine the relation between our results and delocalization-localization transition in the spin-boson model; notably, we point out that a reentrant transition can occur in the regimes where the coupling strength becomes the dominant energy scale. We also discuss applications of our results to other problems in different fields, including quantum optics, condensed matter physics, and quantum chemistry.