Cavity Lifetime Research Articles

Dichroic cavity mode splitting and lifetimes from interactions with a ferromagnetic metal

Dichroic cavity mode splitting and lifetimes from interactions with a ferromagnetic metal

Quantum cascade lasers as broadband sources via strong RF modulation

In this work, we demonstrate that in a regime of strong modulation, by generating pulses of the length of the order of a few cavity lifetimes (hundreds of ps), a broadband quantum cascade laser can be driven to lase on a bandwidth (250 cm−1) limited by the gain. In addition, the amplitude noise of the radiation was shown to be limited by the detector. A laser linewidth study has been performed under different operating conditions, finding values spanning from 20 to 800 MHz, indicating a trade-off between emission bandwidth, amplitude stability, and coherence. The pulsed intensity of the output arises from the gain switching dynamics of the laser, while the self-seeded nature of the emission is responsible for the low amplitude noise and the relatively narrow linewidth of the individual spectral lines of the multimode emission.

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.

Multi-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling

Exciton transport can be enhanced in the strong coupling regime where excitons hybridize with confined light modes to form polaritons. Because polaritons have group velocity, their propagation should be ballistic and long-ranged. However, experiments indicate that organic polaritons propagate in a diffusive manner and more slowly than their group velocity. Here, we resolve this controversy by means of molecular dynamics simulations of Rhodamine molecules in a Fabry-Pérot cavity. Our results suggest that polariton propagation is limited by the cavity lifetime and appears diffusive due to reversible population transfers between polaritonic states that propagate ballistically at their group velocity, and dark states that are stationary. Furthermore, because long-lived dark states transiently trap the excitation, propagation is observed on timescales beyond the intrinsic polariton lifetime. These insights not only help to better understand and interpret experimental observations, but also pave the way towards rational design of molecule-cavity systems for coherent exciton transport.

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.

Coherent qubit measurement in cavity-transmon quantum systems

A measurement of the time between quantum jumps implies the capability to measure the next jump. During the time between jumps the quantum system is not evolving in a closed or unitary manner. While the wave function maintains phase coherence it evolves according to a non-Hermitian effective Hamiltonian. So under null measurement the timing of the next quantum jump can change by very many orders of magnitude when compared to rates obtained by multiplying lifetimes with occupation probabilities obtained via unitary transformation. The theory developed in 1987 for atomic fluorescence is here extended to transitions in transmon qubits. These systems differ from atoms in that they are read out with a harmonic cavity whose resonance is determined by the state of the qubit. We extend our analysis of atomic fluorescence to this infinite level system by treating the cavity as a quantum system. We find that next photon statistics is highly nonexponential and when implemented will enable faster readout, such as on timescales shorter than the decay time of the cavity. Commonly used heterodyne measurements are applied on timescales longer than the cavity lifetime. The overlap between the next photon theory and the theory of heterodyne measurement which are described according to the stochastic Schr\"odinger equation is elucidated. In the limit of large dispersion the intrinsic error for next jump detection, at short time, tends to zero. Whereas for short-time dyne detection the error remains finite for all values of dispersion.

40.1-GHz sub-freezing 850-nm VCSEL: microwave extraction of cavity lifetimes and small-signal equivalent circuit modeling.

We present an 850-nm vertical-cavity surface-emitting laser (VCSEL) constructed for a wide operating temperature range from 25°C to -50°C sub-freezing temperature, demonstrating 40.1-GHz at -50°C. The optical spectra, junction temperature, and microwave equivalent circuit modeling of a sub-freezing 850-nm VCSEL between -50°C and 25°C are also discussed. Reduced optical losses, higher efficiencies, and shorter cavity lifetimes at sub-freezing temperatures are the leading causes of the improved laser output powers and bandwidths. The e-h recombination lifetime and the cavity photon lifetime are shortened to 113 and 4.1 ps, respectively. Could potentially supercharge VCSEL-based sub-freezing optical links for applications in frigid weather, quantum computing, sensing, aerospace, etc.

Non‐Equilibrium Bose–Einstein Condensation of Exciton‐Polaritons in Silicon Metasurfaces

AbstractExciton‐polaritons (EPs) are hybrid light–matter quasi‐particles with bosonic character formed by the strong coupling between excitons in matter and photons in optical cavities. Their hybrid character offers promising prospects for the realization of non‐equilibrium Bose–Einstein condensates (BECs), and room‐temperature BECs are possible with organic materials. However, the thresholds required to create BECs of organic EPs remain still high to allow condensation with electrical injection of carriers. One of the factors behind these high thresholds is the very short cavity lifetimes, leading to a fast EP decay and the need to inject higher exciton densities in the reservoir to form the condensate. Here a BEC of EPs in organic dyes and all‐dielectric metasurfaces at room temperature is demonstrated. By using dielectric metasurfaces that exhibit very low losses it is possible to achieve cavity lifetimes long enough to allow an efficient population of EP states via vibrational relaxation and radiative pumping. It is shown how polariton lasing or non‐equilibrium Bose–Einstein condensation is achieved in several cavities, and one of the lowest reported thresholds for BECs in organic materials is observed.

Experimental study on the transmission characteristics of near-field detonation noise into water

To study the transmission characteristics of near-field detonation noise into water, the detonation noise transmission system is built on a laboratory-scale water tank using a detonation tube with a diameter of 30 mm. The interaction of the detonation gas jet with the air–water interface, the development of the cavity, and the growth of the liquid column are experimentally observed by a high-speed camera. The spectral distribution characteristics of detonation noise above and below the interface are recorded by a microphone, a hydrophone, and an underwater blast sensor. Analysis of the experimental images shows that the size of the cavity increases with increasing filling pressure and decreases with increasing nozzle height. By normalizing the evolution time of the cavity with the cavity lifetime, it is concluded that the time for the cavity to develop to the deepest is about 0.27, independent of the filling pressure. The pressure field data analysis results show that the main frequencies of the detonation sound waves are 100 and 400 Hz, and the frequency distribution has nothing to do with the filling pressure. Through the defined acoustic wave energy transmission coefficient, it is demonstrated that the detonation acoustic wave transmission coefficient decreases with the increase in the frequency, and the shock wave transmission coefficient decreases with the increase in the angle.

Manipulating cavity photon dynamics by topologically curved space

Asymmetric microcavities supporting Whispering-gallery modes (WGMs) are of great significance for on-chip optical information processing. We establish asymmetric microcavities on topologically curved surfaces, where the geodesic light trajectories completely reconstruct the cavity mode features. The curvature-mediated photon-lifetime engineering enables the enhancement of the quality factors of periodic island modes by up to 200 times. Strong and weak coupling between modes of very different origins occurs when the space curvature brings them into resonance, leading to fine tailoring of the cavity photon energy and lifetime and the observation of non-Hermitian exceptional point (EP). At large space curvatures, the role of the WGMs is replaced by high-Q periodic modes protected by the high stability of island-like light trajectory. Our work demonstrates interesting physical mechanisms at the crosspoint of optical chaotic dynamics, non-Hermitian physics, and geodesic optical devices, and would initiate the novel area of geodesic microcavity photonics.

Large Single-Phonon Optomechanical Coupling Between Quantum Dots and Tightly Confined Surface Acoustic Waves in the Quantum Regime

Surface acoustic waves (SAWs) coupled to quantum dots (QDs), trapped atoms and ions, and point defects have been proposed as quantum transduction platforms, yet the requisite coupling rates and cavity lifetimes have not been experimentally established. Although the interaction mechanism varies, small acoustic cavities with large zero-point motion are required for high efficiencies. We experimentally establish the feasibility of this platform through electro- and optomechanical characterization of tightly focusing, single-mode Gaussian SAW cavities at approximately 3.6 GHz on $\mathrm{Ga}\mathrm{As}$. We explore the performance limits of the platform by fabricating SAW cavities with mode volumes approaching $6{\ensuremath{\lambda}}^{3}$ and linewidths less than 1 MHz. Employing strain-coupled single $\mathrm{In}\mathrm{As}$ QDs as optomechanical intermediaries, we measure single-phonon optomechanical coupling rates ${g}_{0}\ensuremath{\approx}2\ensuremath{\pi}\ifmmode\times\else\texttimes\fi{}1.2$ MHz. Sideband scattering rates thus exceed intrinsic phonon loss, indicating the potential for quantum optical readout and transduction of cavity phonon states. To demonstrate the feasibility of this platform for low-noise ground-state quantum transduction, we develop a fiber-based confocal microscope in a dilution refrigerator and perform single-QD resonance fluorescence sideband spectroscopy at millikelvin temperatures. These measurements show conversion between microwave phonons and optical photons with sub-natural linewidths.

Coronal Cavities in CoMP Observations

Abstract Quiescent coronal cavities can provide insight into solar magnetic fields. They are observed in the coronal emission lines in both polarized and unpolarized light. In the total linear polarization fraction (L/I), they often possess a “lagomorphic,” or “rabbit-shaped,” structure that reflects the underlying magnetic field configuration. We studied quiescent coronal cavities observed between 2012 and 2018 by the Coronal Multichannel Polarimeter (CoMP). The majority of cavities in our study had a characteristic lagomorphic structure in linear polarization. We additionally compared cavity widths as observed in intensity with sizes of their linear polarization signatures for 70 cavities and found that both features are strongly correlated. Our results indicate that chances for observing a lagomorphic structure increase greatly with cavity lifetime, suggesting that the visibility depends on the spatial orientation of the cavity. Forward-modeled observations in linear polarization of flux ropes confirmed this assumption. We conclude that observations of the solar coronal cavities in linear polarization are consistent with the theoretical model of flux rope formation and structure.

Nonequilibrium mode competition in a pumped dye-filled cavity

We consider a homogeneously pumped photon gas coupled to a dye medium and investigate how its steady state is effected when varying the pump power, the photon cavity lifetime and the cutoff frequency. We study how the interplay between pumping, loss, and dye-induced thermalization influences the selection of the cavity modes that acquire large occupation. Depending on the parameter regime, the latter can be related either to lasing of (typically multiple) modes or to equilibrium-like photon condensation in the ground mode. We calculate and explain the phase diagram of the system, with a particular emphasis on the role played by a mode repulsion that occurs in the regime of weak cavity loss.

Photon Conversion and Interaction in a Quasi-Phase-Matched Microresonator

The conversion and interaction between quantum signals at the single-photon level are essential for scalable quantum photonic information technology. Using a fully optimized periodically poled lithium niobate microring, we demonstrate ultraefficient sum-frequency generation on a chip. The external quantum efficiency reaches $(65\ifmmode\pm\else\textpm\fi{}3)\mathrm{%}$ with only $(104\ifmmode\pm\else\textpm\fi{}4)$-$\ensuremath{\mu}\mathrm{W}$ pump power. At peak conversion, $3\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}5}$-noise photon is created during the cavity lifetime, which meets the requirement of quantum applications using single-photon pulses. Using a pump and signal in single-photon coherent states, we directly measure the conversion probability produced by a single pump photon to be ${10}^{\ensuremath{-}5}$, which is a significant improvement from the state of the art, and the photon-photon coupling strength to be 9.1 MHz. Our results mark steady progress toward quantum nonlinear optics at the ultimate single-photon limit, with potential applications in highly integrated photonics and quantum optical computing.

Stabilizing nanolasers via polarization lifetime tuning

We investigate the emission dynamics of mutually coupled nanolasers and predict ways to optimize their stability, i.e., maximize their locking range. We find that tuning the cavity lifetime to the same order of magnitude as the dephasing time of the microscopic polarization yields optimal operation conditions, which allow for wider tuning ranges than usually observed in conventional semiconductor lasers. The lasers are modeled by Maxwell–Bloch type class-C equations. For our analysis, we analytically determine the steady state solutions, analyze the symmetries of the system and numerically characterize the emission dynamics via the underlying bifurcation structure. The polarization lifetime is found to be a crucial parameter, which impacts the observed dynamics in the parameter space spanned by frequency detuning, coupling strength and coupling phase.

Effect of Surface Recombination on Diffusion Length and Active Cavity Life time

This work presents an analytical study for simulating a Fabry-Perot Bi-stable etalon (F-P cavity) filled with a dispersive optimized nonlinear optical material (Kerr type) such as semiconductors Indium Antimonite (InSb). Depending on the obtained results and because of a trade-off between the optical path length of the sample and active cavity lifetime, an optimization procedure was applied on the InSb etalon/CO laser parameters; critical switching irradiance (Ic) was applied via simulation systems of optimization procedures of optical cavity (Matlap program was used to study the optical Bi-stability of a nonlinear Fabry-Perot cavity). In order to achieve minimum switching power and faster switching time, the optimization surface recombination on the diffusion length and effective cavity lifetime was studied.
 In addition, for a specific absorption value 400 cm-1, the lifetime coefficient values were 0.33 , 0.091 , 0.0172 ns for sample thickness (D) = 500 , 60 , 20 mm, respectively. Also, for a bulk recombination time (Tl) of 200 ns, specific absorption (α) of 50 cm1, and D of 20 mm, the surface recombination speed value was 2.845 x 105 cm/sec, whereas the active lifetime, which is defined as the thickness over the surface recombination speed (sυ) (D/2sυ), was equal to 3.5ns.

Dynamics and spectroscopy of molecular ensembles in a lossy microcavity.

The radiative and nonradiative relaxation dynamics of an ensemble of molecules in a microcavity are investigated with emphasis on the impact of the cavity lifetime on reactive and spectroscopic properties. Extending a previous study [I. S. Ulusoy et al., J. Phys. Chem. A 123, 8832-8844 (2019)], it is shown that the dynamics of the ensemble and of single molecules are influenced by the presence of a cavity resonance as long as the polariton splitting can be resolved spectroscopically, which critically depends on the lifetime of the system. Our simulations illustrate how the branching between nonradiative intersystem crossing and radiative decay through the cavity can be tuned by selecting specific cavity photon energies resonant at specific molecular geometries. In the case of cavity-photon energies that are not resonant at the Franck-Condon geometry of the molecules, it is demonstrated numerically and analytically that collective effects are limited to a handful of molecules in the ensemble.

Atypical vibrational interactions

Chemical Physics Vibrational energy transfer (VET) between solute molecules is generally unfavorable in liquids because of weak intermolecular forces. Xiang et al. measured the two-dimensional infrared spectrum of a molecular mixture, W(CO)6 and W(13CO)6, with saturated concentrations in a binary solvent embedded in an optical microcavity. This experiment showed that the VET between the asymmetric stretch vibrations of two solute molecules is enhanced via polaritonic intermediate states formed by a strong coupling with the cavity mode. The efficiency is modulated by the cavity lifetime, which provides an opportunity to control the VET process in the liquid phase. This could lead to various practical implementations. Science , this issue p. [665][1] [1]: /lookup/doi/10.1126/science.aba3544

Intermolecular vibrational energy transfer enabled by microcavity strong light-matter coupling.

Selective vibrational energy transfer between molecules in the liquid phase, a difficult process hampered by weak intermolecular forces, is achieved through polaritons formed by strong coupling between cavity photon modes and donor and acceptor molecules. Using pump-probe and two-dimensional infrared spectroscopy, we found that the excitation of the upper polariton, which is composed mostly of donors, can efficiently relax to the acceptors within ~5 picoseconds. The energy-transfer efficiency can be further enhanced by increasing the cavity lifetime, suggesting that the energy transfer is a polaritonic process. This vibrational energy-transfer pathway opens doors for applications in remote chemistry, sensing mechanisms, and vibrational polariton condensation.

Tracking Polariton Relaxation with Multiscale Molecular Dynamics Simulations.

When photoactive molecules interact strongly with confined light modes in optical cavities, new hybrid light–matter states form. They are known as polaritons and correspond to coherent superpositions of excitations of the molecules and of the cavity photon. The polariton energies and thus potential energy surfaces are changed with respect to the bare molecules, such that polariton formation is considered a promising paradigm for controlling photochemical reactions. To effectively manipulate photochemistry with confined light, the molecules need to remain in the polaritonic state long enough for the reaction on the modified potential energy surface to take place. To understand what determines this lifetime, we have performed atomistic molecular dynamics simulations of room-temperature ensembles of rhodamine chromophores strongly coupled to a single confined light mode with a 15 fs lifetime. We investigated three popular experimental scenarios and followed the relaxation after optically pumping (i) the lower polariton, (ii) the upper polariton, or (iii) uncoupled molecular states. The results of the simulations suggest that the lifetimes of the optically accessible lower and upper polaritons are limited by (i) ultrafast photoemission due to the low cavity lifetime and (ii) reversible population transfer into the “dark” state manifold. Dark states are superpositions of molecular excitations but with much smaller contributions from the cavity photon, decreasing their emission rates and hence increasing their lifetimes. We find that population transfer between polaritonic modes and dark states is determined by the overlap between the polaritonic and molecular absorption spectra. Importantly, excitation can also be transferred ”upward” from the lower polariton into the dark-state reservoir due to the broad absorption spectra of the chromophores, contrary to the common conception of these processes as a ”one-way” relaxation from the dark states down to the lower polariton. Our results thus suggest that polaritonic chemistry relying on modified dynamics taking place within the lower polariton manifold requires cavities with sufficiently long lifetimes and, at the same time, strong light–matter coupling strengths to prevent the back-transfer of excitation into the dark states.