Optomechanical systems are a promising candidate for the implementation of quantum interfaces for storing and redistributing quantum information. Here we focus on the case of a high-finesse optical cavity with a thin vibrating semitransparent membrane in the middle. We show that robust and stationary optomechanical entanglement could be achieved in the system, even in the presence of nonnegligible optical absorption in the membrane. We also present some preliminary experimental data showing radiation-pressure induced optical bistability.
We study the cavity mode frequencies of a Fabry-Pérot cavity containing two vibrating dielectric membranes. We derive the equations for the mode resonances and provide approximate analytical solutions for them as a function of the membrane positions, which act as an excellent approximation when the relative and center-of-mass position of the two membranes are much smaller than the cavity length. With these analytical solutions, one finds that extremely large optomechanical coupling of the membrane relative motion can be achieved in the limit of highly reflective membranes when the two membrane…
We study the quantum dynamics of the cavity optomechanical system formed by a Fabry-Perot cavity with a thin vibrating membrane at its center. We first derive the general multimode Hamiltonian describing the radiation pressure interaction between the cavity modes and the vibrational modes of the membrane. We then restrict the analysis to the standard case of a single cavity mode interacting with a single mechanical resonator and we determine to what extent optical absorption by the membrane hinder reaching a quantum regime for the cavity-membrane system. We show that membrane absorption does n…
We present an experimental study of an optomechanical system formed by a vibrating thin semi-transparent membrane within a high-finesse optical cavity. We show that the coupling between the optical cavity modes and the vibrational modes of the membrane can be tuned by varying the membrane position and orientation. In particular we demonstrate a large quadratic dispersive optomechanical coupling in correspondence with avoided crossings between optical cavity modes weakly coupled by scattering at the membrane surface. The experimental results are well explained by a first order perturbation trea…
Strong coupling of molecular vibrations to an infrared cavity mode affects their nature by creating dressed polariton states. We show how the single and double vibrational polariton manifolds may be controlled by varying the cavity coupling strength, and probed by a time domain 2DIR technique, Double Quantum Coherence (DQC). Applications are made to the amide-I ($CO$) and amide-II ($CN$) bond vibrations of $N-methylacetamide$ (NMA).
We describe a cryogenic cavity-optomechanical system that combines Si3N4 membranes with a mechanically-rigid Fabry-Perot cavity. The extremely high quality-factor frequency products of the membranes allow us to cool a MHz mechanical mode to a phonon occupation of less than 10, starting at a bath temperature of 5 kelvin. We show that even at cold temperatures thermally-occupied mechanical modes of the cavity elements can be a limitation, and we discuss methods to reduce these effects sufficiently to achieve ground state cooling. This promising new platform should have versatile uses for hybrid …
We present an experimental study of dynamical back-action cooling of the fundamental vibrational mode of a thin semitransparent membrane placed within a high-finesse optical cavity. We study how the radiation pressure interaction modifies the mechanical response of the vibrational mode, and the experimental results are in agreement with a Langevin equation description of the coupled dynamics. The experiments are carried out in the resolved sideband regime, and we have observed cooling by a factor 350 We have also observed the mechanical frequency shift associated with the quadratic term in the…
Optomechanical arrays made of structured flexible dielectrics are a promising system for exploring quantum and many-body optomechanical phenomena. We generalize investigations of the optomechanical properties of periodic arrays of one-dimensional scatterers in optical resonators to the case of vibrating membranes whose thickness is not necessarily small with respect to the optical wavelength of interest. The array optical transmission spectrum and its optomechanical coupling with a linear Fabry-Perot cavity field are investigated both analytically and numerically.
We demonstrate the analogue of electromagnetically induced transparency in a room temperature cavity optomechanics setup formed by a thin semitransparent membrane within a Fabry-Pérot cavity. Due to destructive interference, a weak probe field is completely reflected by the cavity when the pump beam is resonant with the motional red sideband of the cavity. Under this condition we infer a significant slowing down of light of hundreds of microseconds, which is easily tuned by shifting the membrane along the cavity axis. We also observe the associated phenomenon of electromagnetically induced amp…
We demonstrate feedback cooling of a millimeter-scale, 40 kHz SiN membrane from room temperature to 5 mK (3000 phonons) using a Michelson interferometer, and discuss the challenges to ground state cooling without an optical cavity. This advance appears within reach of current membrane technology, positioning it as a compelling alternative to levitated systems for quantum sensing and fundamental weak force measurements.
We present a scheme to entangle the vibrational phonon modes of two massive ferromagnetic spheres in a dual-cavity magnomechanical system. In each cavity, a microwave cavity mode couples to a magnon mode (spin wave) via the magnetic dipole interaction, and the latter further couples to a deformation phonon mode of the ferromagnetic sphere via a nonlinear magnetostrictive interaction. We show that by directly driving the magnon mode with a red-detuned microwave field to activate the magnomechanical anti-Stokes process a cavity-magnon-phonon state-swap interaction can be realized. Therefore, if …
We propose a method to generate entangled states of the vibrational modes of N membranes which are coupled to a cavity mode via the radiation pressure. Using sideband excitations, we show that arbitrary entangled states of vibrational modes of different membranes can be produced in principle by sequentially applying a series of classical pulses with desired frequencies, phases and durations. As examples, we show how to synthesize several typical entangled states, for example, Bell states, NOON states, GHZ states and W states. The environmental effect, information leakage, and experimental feas…
We investigate the optomechanical properties of tensile-strained ternary InGaP nanomembranes grown on GaAs. This material system combines the benefits of highly strained membranes based on stoichiometric silicon nitride, with the unique properties of thin-film semiconductor single crystals, as previously demonstrated with suspended GaAs. Here we employ lattice mismatch in epitaxial growth to impart an intrinsic tensile strain to a monocrystalline thin film (approximately 30 nm thick). These structures exhibit mechanical quality factors of 2*10^6 or beyond at room temperature and 17 K for eigen…
We study the optomechanical behaviour of a driven Fabry-Pérot cavity containing two vibrating dielectric membranes. We characterize the cavity-mode frequency shift as a function of the two-membrane positions, and report a $\sim 2.47$ gain in the optomechanical coupling strength of the membrane relative motion with respect to the single membrane case. This is achieved when the two membranes are properly positioned to form an inner cavity which is resonant with the driving field. We also show that this two-membrane system has the capability to tune the single-photon optomechanical coupling on de…
We investigate a dual membrane active-passive cavity where each mechanical membrane individually quadratically coupled to passive and active cavities via two-phonon process. Due to the fact that in the quadratically coupled optomechanical system mean-field approximation fails, hence to analyze the system completely, we switch to a more generalized out of equilibrium approach, namely Keldysh Green's functional approach. We calculate transmission rate using predetermined full retarded Green's function, and then numerically examine the effect of the various parameters on the transmission coeffici…
The optical hybridization of the electronic states in strongly coupled molecule-cavity systems have revealed unique properties such as lasing, room temperature polariton condensation, and the modification of excited electronic landscapes involved in molecular isomerization. Here we show that molecular vibrational modes of the electronic ground state can also be coherently coupled with a micro-cavity mode at room temperature, given the low vibrational thermal occupation factors associated with molecular vibrations, and the collective coupling of a large ensemble of molecules immersed within the…
We discuss a hybrid quantum system where a dielectric membrane situated inside an optical cavity is coupled to a distant atomic ensemble trapped in an optical lattice. The coupling is mediated by the exchange of sideband photons of the lattice laser, and is enhanced by the cavity finesse as well as the square root of the number of atoms. In addition to observing coherent dynamics between the two systems, one can also switch on a tailored dissipation by laser cooling the atoms, thereby allowing for sympathetic cooling of the membrane. The resulting cooling scheme does not require resolved sideb…
We formulate a non-relativistic Hamiltonian in order to describe the interaction between a moving dielectric membrane and radiation pressure. Such a Hamiltonian is derived without making use of the single-mode adiabatic approximation, and hence it enables us to incorporate multi-mode effects in cavity optomechanics. By performing second quantization, we show how a set of generalized Fock states can be constructed to represent quantum states of the membrane and cavity field. In addition, we discuss examples showing how photon scattering among different cavity modes would modify the interaction …
We investigate theoretically the extension of cavity optomechanics to multiple membrane systems. We describe such a system in terms of the coupling of the collective normal modes of the membrane array to the light fields. We show these modes can be optically addressed individually and be cooled, trapped and characterized, e.g. via quantum nondemolition measurements. Analogies between this system and a linear chain of trapped ions or dipolar molecules imply the possibility of related applications in the quantum regime.
We present the results of theoretical and experimental studies of dispersively coupled (or "membrane in the middle") optomechanical systems. We calculate the linear optical properties of a high finesse cavity containing a thin dielectric membrane. We focus on the cavity's transmission, reflection, and finesse as a function of the membrane's position along the cavity axis and as a function of its optical loss. We compare these calculations with measurements and find excellent agreement in cavities with empty-cavity finesses in the range 10^4 to 10^5. The imaginary part of the membrane's index o…
We propose a theoretical scheme to show the possibility of generating motional nonlinear coherent states and their superposition for an undamped vibrating micromechanical membrane inside an optical cavity. The scheme is based on an intensity-dependent coupling of the membrane to the radiation pressure field. We show that if the cavity field is initially prepared in a Fock state, the motional state of the membrane may evolve from vacuum state to a special type of nonlinear coherent states. By examining the nonclassical properties of the generated state of the membrane, including the quadrature …
A scheme is presented for the adiabatic transfer of average fluctuation in the phonon number between two membranes in an optical cavity. We show that by driving the cavity modes with external time-delayed pulses, one can obtain an effect analogous to stimulated Raman adiabatic passage (STIRAP) in the atomic systems. In this adiabatic processes the population is trapped between two states by creating a dark state.The adiabatic transfer of fluctuation from one membrane to the other is attained through a 'dark' mode, that is robust against decay of the mediating cavity mode.The results are suppor…
In this paper, by invariant-based inverse engineering, we design classical driving fields to transfer quantum fluctuations between two suspended membranes in an optomechanical cavity system. The transfer can be quickly attained through a non-adiabatic evolution path determined by a so-called dynamical invariant. Such an evolution path allows one to optimize the occupancies of the unstable "intermediate" states thus the influence of cavity decays can be suppressed. Numerical simulation demonstrates that a perfect fluctuation transfer between two membranes can be rapidly achieved in one step, an…
We demonstrate a cryogenic optomechanical system comprising a flexible Si3N4 membrane placed at the center of a free-space optical cavity in a 400 mK cryogenic environment. We observe a mechanical quality factor Q > 4 x 10^6 for the 261-kHz fundamental drum-head mode of the membrane, and a cavity resonance halfwidth of 60 kHz. The optomechanical system therefore operates in the resolved sideband limit. We monitor the membrane's thermal motion using a heterodyne optical circuit capable of simultaneously measuring both of the mechanical sidebands, and find that the observed optical spring and da…
We study the non-linear dynamics of a multimode optomechanical system constituted of a driven high-finesse Fabry-Pérot cavity containing two vibrating dielectric membranes. The analytical study allows to derive a full and consistent description of the displacement detection by a probe beam in the non-linear regime, enabling the faithful detection of membrane displacements well above the usual sensing limit corresponding to the cavity linewidth. In the weak driving regime where the system is in a pre-synchronized situation, the unexcited oscillator has a small, synchronized component at the fre…
While the emerging field of vibrational polariton chemistry has the potential to overcome traditional limitations of synthetic chemistry, the underlying mechanism is not yet well understood. Here, we explore how the dynamics of unimolecular dissociation reactions that are rate-limited by intramolecular vibrational energy redistribution (IVR) can be modified inside an infrared optical cavity. We study a classical model of a bent triatomic molecule, where the two outer atoms are bound by anharmonic Morse potentials to the center atom coupled to a harmonic bending mode. We show that an optical ca…
Macroscopic mechanical objects and electromagnetic degrees of freedom couple to each other via radiation pressure. Optomechanical systems with sufficiently strong coupling are predicted to exhibit quantum effects and are a topic of considerable interest. Devices reaching this regime would offer new types of control of the quantum state of both light and matter and would provide a new arena in which to explore the boundary between quantum and classical physics. Experiments to date have achieved sufficient optomechanical coupling to laser-cool mechanical devices but have not yet reached the quan…
We realize a potential platform for an efficient spin-photon interface, namely negatively-charged silicon-vacancy centers in a diamond membrane coupled to the mode of a fully-tunable, fiber-based, optical resonator. We demonstrate that introducing the thin ($\sim 200 \, \text{nm}$), single crystal diamond membrane into the mode of the resonator does not change the cavity properties, which is one of the crucial points for an efficient spin-photon interface. In particular, we observe constantly high Finesse values of up to $3000$ and a linear dispersion in the presence of the membrane. We observ…
We propose a cavity QED approach to describe light-matter interaction between an individual anharmonic molecular vibration and an infrared cavity field. Starting from a generic Morse oscillator with quantized nuclear motion, we derive a multi-level quantum Rabi model to study vibrational polaritons beyond the rotating-wave approximation. We analyze the spectrum of vibrational polaritons in detail and compare with available experiments. For high excitation energies, the spectrum exhibits a dense manifold of true and avoided level crossings as the light-matter coupling strength and cavity freque…
The nitrogen-vacancy center in diamond has been explored extensively as a light-matter interface for quantum information applications, however it is limited by low coherent photon emission and spectral instability. Here, we present a promising interface based on an alternate defect with superior optical properties (the germanium-vacancy) coupled to a finesse $\approx11{,}000$ fiber cavity, resulting in a $31^{+11}_{-15}$-fold increase in the spectral density of emission. This work sets the stage for cryogenic experiments, where we predict a measurable increase in the spontaneous emission rate.
We consider an optomechanical system comprising a single cavity mode and a dense spectrum of acoustic modes and solve for the quantum dynamics of initial cavity mode Fock (i.e., photon number) superposition states and thermal acoustic states. The optomechanical interaction results in dephasing without damping and bears some analogy to gravitational decoherence. For a cavity mode locally coupled to a one-dimensional (1D) elastic string-like environment or two-dimensional (2D) elastic membrane-like environment, we find that the dephasing dynamics depends respectively on the string length and mem…
The interaction between a high-frequency dilational mode of a thin dielectric film and an optical cavity field is studied theoretically in the membrane-in-the-middle setup. A derivation from first principles leads to a multi-mode optomechanical Hamiltonian where multiple cavity modes are coupled by the thickness variation of the membrane. For membrane thicknesses on the order of one micron, the frequency of this dilational mode is in the GHz range. This can be matched to the free spectral range of the optical cavity, such that the mechanical oscillator will resonantly couple cavity modes at di…
We present detailed calculations at the basis of our recent proposal for simultaneous cooling the rotational, vibrational and external molecular degrees of freedom. In this method, the molecular rovibronic states are coupled by an intense laser and an optical cavity via coherent Raman processes enhanced by the strong coupling with the cavity modes. For a prototype system, OH, we showed that the translational motion is cooled to few micro Kelvin and the molecule is brought to the internal ground state in about a second. Here, we investigate numerically the dependence of the cooling scheme on th…
Phonon interactions are inevitable in cavity quantum electrodynamical systems based on solid-state emitters or fluorescent molecules, where vibrations of the lattice or chemical bonds couple to the electronic degrees of freedom. Due to the non-Markovian response of the vibrational environment, it remains a significant theoretical challenge to describe such effects in a computationally efficient manner. This is particularly pronounced when the emitter-cavity coupling is comparable to or larger than the typical phonon energy range, and polariton formation coincides with vibrational dressing of t…
We describe an optomechanical device consisting of a fiber-based optical cavity containing a silicon nitiride membrane. In comparison with typical free-space cavities, the fiber-cavity's small mode size (10 μm waist, 80 μm length) allows the use of smaller, lighter membranes and increases the cavity-membrane linear coupling to 3 GHz/nm and quadratic coupling to 20 GHz/nm^2. This device is also intrinsically fiber-coupled and uses glass ferrules for passive alignment. These improvements will greatly simplify the use of optomechanical systems, particularly in cryogenic settings. At room temperat…
We introduce a passively-aligned, flexure-tuned cavity optomechanical system in which a membrane is positioned microns from one end mirror of a Fabry-Perot optical cavity. By displacing the membrane through gentle flexure of its silicon supporting frame (i.e., to ~80 m radius of curvature (ROC)), we gain access to the full range of available optomechanical couplings, finding also that the optical spectrum exhibits none of the abrupt discontinuities normally found in "membrane-in-the-middle" (MIM) systems. More aggressive flexure (3 m ROC) enables >15 microns membrane travel, milliradian tilt t…
We theoretically demonstrate that chemical reaction rate constant can be significantly suppressed by coupling molecular vibrations with an optical cavity, exhibiting both the collective coupling effect and the cavity-frequency modification of the rate constant. When a reaction coordinate is strongly coupled to the solvent molecules, the reaction rate constant is reduced due to the dynamical caging effect. We demonstrate that collectively coupling the solvent to the cavity can further enhance this dynamical caging effect, leading to additional suppression of the chemical kinetics. This effect i…
We calculate the optomechanical coupling strength for a multi-membrane in a cavity system. The optimal configuration for an array of $N$ membranes placed near the center of a cavity is identified. This results in a coupling strength much greater than previously proposed multi-membrane configurations. We find that the coupling strength scales exponentially with the number of membranes until saturating due to complete localization of the field within the array. Furthermore we explore two sources of loss, those due to light absorption within the membrane(s) and leakage through the cavity's end-mi…
Cavity-optomechanics enables photon-phonon interaction and correlations by harnessing the radiation-pressure force. Here, we realize a ``cavity-in-a-membrane'' optomechanical architecture which allows detection of the motion of lithographically-defined, ultrathin membranes via an integrated optical cavity. Using a dissipative filtering method, we are able to eliminate the probe light in situ and observe photon-phonon correlations associated with the low-frequency membrane mechanical mode. The developed method is generally applicable for study of low-frequency light scattering processes where c…
We consider a quantum optomechanical scheme wherein an ordered two-dimensional array of laser-trapped atoms is used as a movable membrane. The extremely light mass of the atoms yields very strong optomechanical coupling, while their spatial order largely eliminates scattering losses. We show that this combination opens the way for quantum optomechanical nonlinearities, well within the ultimate single-photon strong-coupling regime. As an example, we analyze the possibility to observe optomechanically induced quantum effects such as photon blockade and time-delayed non-classical correlations. We…
We investigate the feasibility of correlating an optical cavity field and a vibrational phonon mode. A laser pumped quantum dot fixed on a nano-mechanical resonator beam interact as a whole with the optical resonator mode. When the quantum dot variables are faster than the optical and phonon ones, we obtain a final master equation describing the involved modes only. Increasing the temperature, that directly affects the vibrational degrees of freedom, one can as well influence the cavity photon intensity, i.e., the optical and phonon modes are correlated. Furthermore, the corresponding Cauchy-S…
We discuss Floquet engineering of dissipative molecular systems through periodic driving of an infrared-active vibrational transition, either directly or via a cavity mode. Following a polaron quantum Langevin equations approach, we derive correlation functions and stationary quantities showing strongly modified optical response of the infrared-dressed molecule. The coherent excitation of molecular vibrational modes, in combination with the modulation of electronic degrees of freedom due to vibronic coupling can lead to both enhanced vibronic coherence as well as control over vibrational sideb…
The electromagnetic field in an optical cavity can dramatically modify and even control chemical reactivity via vibrational strong coupling (VSC). Since the typical vibration and cavity frequencies are considerably higher than thermal energy, it is essential to adopt a quantum description of cavity-catalyzed adiabatic chemical reactions. Using quantum transition state theory (TST), we examine the coherent nature of adiabatic reactions and derive the cavity-induced changes in eigen frequencies, zero-point-energy, and quantum tunneling. The resulting quantum TST calculation allows us to explain …
Spontaneous synchronization is a significant collective behavior of weakly coupled systems. Due to their inherent nonlinear nature, optomechanical systems can exhibit self-sustained oscillations which can be exploited for synchronizing different mechanical resonators. In this paper, we explore the synchronization dynamics of two membranes coupled to a common optical field within a cavity, and pumped with a strong blue-detuned laser drive. We focus on the system quantum dynamics in the parameter regime corresponding to synchronization of the classical motion of the two membranes. With an approp…
We analyse the reaction of a massless (1+1)-dimensional spinor field to the harmonic motion of one cavity wall. In our model, the oscillation amplitude of the harmonic oscillator is promoted to a quantum operator, providing the system with an additional quantum degree of freedom having bosonic nature. After obtaining the interaction Hamiltonian, we estimate the correction to both the ground state and its energy. We demonstrate that the system is able to convert bosons into fermion pairs at the lowest perturbative order. Extension of our model to multiple bags is contemplated.
Spontaneous Raman Scattering under Vibrational Strong Coupling: The Critical Role of Polariton Spatial Mode Coherence
Université de Strasbourg, CNRS, Institut de Physique et Chimie des Matériaux de Strasbourg（斯特拉斯堡大学）；Université Claude Bernard Lyon 1, CNRS, Institut Lumière Matière（里昂第一大学）
In vibrational strong coupling (VSC), molecular vibrations strongly interact with the modes of an optical cavity to form hybrid light-matter states known as vibrational polaritons. Experiments show that the kinetics of thermally activated chemical reactions can be modified by VSC. Transition-state theory, which assumes that internal thermalization is fast compared to reactive transitions, has been unable to explain the observed findings. Here, we carry out kinetic simulations to understand how dissipative processes, namely those that VSC introduces to the chemical system, affect reactions wher…
