We present a scheme to realize precise discrimination of chiral molecules in a cavity. Assisted by additional laser pulses, cavity fields can evolve to different coherence states with contrary-sign displacements according to the handedness of molecules. Consequently, the handedness of molecules can be read out with homodyne measurement on the cavity, and the successful probability is nearly unity without very strong cavity fields. Numerical results show that the scheme is insensitive to errors, noise and decoherence. Therefore, the scheme may provide helpful perspectives for accurate discrimination of chiral molecules.
We propose an oversimplified scheme to unambiguously discriminate nonorthogonal quantum field states inside high-Q cavities. Our scheme, which is based on positive operator-valued mea- sures (POVM) technique, uses a single three-level atom interacting resonantly with a single mode of a cavity-field and selective atomic state detectors. While the single three-level atom takes the role of the ancilla, the single cavity mode field represents the system we want to obtain information. The efficiency of our proposal is analyzed considering the nowadays achievements in the context of cavity QED.
We consider the problem of discriminating macromolecular structures in an electron microscope, through a specific beam shaping technique. Our approach is based on maximizing the which-molecule information extracted from the state of each electron. To this aim, the optimal observables are derived within the framework of quantum state discrimination, which allows one to fully account from the quantum character of the probe. We simulate the implementation of such optimal observable on a generalized orbital angular momentum (OAM) sorter and benchmark its performance against the best known real spa…
We propose to discriminate chiral molecules by combining one- and two-photon processes in a closed-loop configuration. The one-photon-coupling intrinsic π-phase difference between two enantiomers leads to their different superposition states, which is then followed by a two-photon process through three-mode parallel paths (3MPPs), enabling the discrimination of enantiomers by inducing their entirely-different population distributions. The 3MPPs are constructed by "chosen paths", a method of shortcuts to adiabaticity (STA), exhibiting a fast two-photon process. As an example, we propose to perf…
Resonance energy transfer between chiral molecules can be used to discriminate between different enantiomers. The transfer rate between chiral molecules consists of a non-discriminatory and discriminatory parts. We derive these two rate contributions in the framework of macroscopic quantum electrodynamics. We show that their ratio is usually larger in the retarded regime or far-zone of large separation distances and that the degree of discrimination can be modified when considering a surrounding medium. We highlight the importance of local field effects onto the degree of discrimination and pr…
A general scheme for rotational cooling of diatomic heteronuclear molecules is proposed. It uses a superconducting microwave cavity to enhance the spontaneous decay via Purcell effect. Rotational cooling can be induced by sequentially tuning each rotational transition to cavity resonance, starting from the highest transition level to the lowest using an electric field. Electrostatic multipoles can be used to provide large confinement volume with essentially homogeneous background electric field.
A cavity quantum electrodynamical scenario is proposed for implementing a Schrödinger microscope capable of amplifying differences between non orthogonal atomic quantum states. The scheme involves an ensemble of identically prepared two-level atoms interacting pairwise with a single mode of the radiation field as described by the Tavis-Cummings model. By repeated measurements of the cavity field and of one atom within each pair a measurement-induced nonlinear quantum transformation of the relevant atomic states can be realized. The intricate dynamical properties of this nonlinear quantum trans…
Cavity cooling of an atom works best on a cyclic optical transition in the strong coupling regime near resonance, where small cavity photon numbers suffice for trapping and cooling. Due to the absence of closed transitions a straightforward application to molecules fails: optical pumping can lead the particle into uncoupled states. An alternative operation in the far off-resonant regime generates only very slow cooling due to the reduced field-molecule coupling. We predict to overcome this by using a strongly driven ring-cavity operated in the sideband cooling regime. As in the optomechanical …
We analyze cavity-assisted cooling schemes for polar molecules in the microwave domain, where molecules are excited on a rotational transition and energy is dissipated via strong interactions with a lossy stripline cavity, as recently proposed by A. Andre et al., Nature Physics 2, 636 (2006). We identify the dominant cooling and heating mechanisms in this setup and study cooling rates and final temperatures in various parameter regimes. In particular we analyze the effects of a finite environment temperature on the cooling efficiency, and find minimal temperature and optimized cooling rate in …
A dressed-state perturbation theory beyond the rotating waveapproxi-mation (RWA) is presented to investigate the interaction between a two level electronic transition of the polar molecules and a quantized cavity field. Analytical expressions can be explicitly derived for both the ground- and excited-state-energy spectrums and wave functions of the system, where the contribution of permanent dipole moments (PDM) and the counter-rotating wave term (CRT) can be shown separately. The validity of these explicit results is discussed by comparing with the direct numerical simulation. Comparing to CR…
Plasmonic dimer cavities can induce extreme electric-field hot spots that allow one to access ultrastrong coupling regimes using Raman-type spectroscopy on single vibrating molecules. Using a generalized master equation, we study resonant Raman scattering in the strong coupling regime of cavity-QED, when also in the vibrational ultrastrong coupling regime, leading to "phonon-dressed polaritons". The master equation rigorously includes spectral baths for the cavity and vibrational degrees of freedom, as well as a pure dephasing bath for the resonant two-level system, which play a significant ro…
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…
We analyze the thermal Casimir-Polder potential experienced by a ground-state molecule in a planar cavity and investigate the prospects for using such a set-up for molecular guiding. The resonant atom-field interaction associated with this non-equilibrium situation manifests itself in oscillating, standing-wave components of the potential. While the respective potential wells are normally too shallow to be useful, they may be amplified by a highly reflecting cavity whose width equals a half-integer multiple of a particular molecular transition frequency. We find that with an ideal choice of mo…
The decay rate and the classical radiation power of an excited molecule (atom) located in the center of a dispersive and absorbing dielectric sphere taken as a simple model of a cavity are calculated adopting the Onsager model for the local field. The local-field correction factor to the external (radiation and absorption) power loss of the molecule is found to be $|3ε(ω)/[3ε(ω)+1]|^2$, with $ε(ω)$ being the dielectric function of the sphere. However, local-field corrections to the total decay rate (power loss) of the molecule are found to be much more complex, including those to the decay rat…
We theoretically study non-destructive detection of ultracold molecules, using a Fabry-Perot cavity. Specifically, we consider vacuum Rabi splitting where we demonstrate the use of collective strong coupling for detection of molecules with many participating energy levels. We also consider electromagnetically induced transparency and transient response of light for the molecules interacting with a Fabry-Perot cavity mode, as a mean for non-destructive detection. We identify the parameters that are required for the detection of molecules in the cavity electromagnetically induced transparency co…
In recent studies [Liew et al., Phys. Rev. Lett. 104, 183601 (2010); Bamba et al., Phys. Rev. A 83, 021802(R) (2011)], due to destructive interference between different paths for two-photon excitation, strong photon antibunching can be obtained in a photonic molecule consisting of two coupled cavity modes with weak Kerr nonlinearity when one of the cavity modes is driven resonantly. Here, we study the photon statistics in a nonlinear photonic molecule with both the two cavity modes being driven coherently. We show that the statistical properties of the photons can be controlled by regulating t…
We demonstrate the effects of cavity quantum electrodynamics for a quantum dot coupled to a photonic molecule, consisting of a pair of coupled photonic crystal cavities. We show anti-crossing between the quantum dot and the two super-modes of the photonic molecule, signifying achievement of the strong coupling regime. From the anti-crossing data, we estimate the contributions of both mode-coupling and intrinsic detuning to the total detuning between the super-modes. Finally, we also show signatures of off-resonant cavity-cavity interaction in the photonic molecule.
Cooling a range of molecules to ultracold temperatures (<1 mK) is a difficult but important challenge in molecular physics and chemistry. Collective cavity cooling of molecules is a promising method that does not rely on molecular energy level and thus can be applied to all molecules in principle. However, the initial lack of cold molecules leads to the difficulty in its experimental implementation. We show that efficient collective sympathetic cooling of molecules to sub-mK temperatures using a large ensemble of atoms within a cavity is feasible. This approach is a new type of sympathetic coo…
We derive a master equation for the motion of a polarizable particle weakly interacting with one or several strongly pumped cavity modes. We focus here on massive particles with complex internal structure such as large molecules and clusters, for which we assume a linear scalar polarizability mediating the particle-light interaction. The predicted friction and diffusion coefficients are in good agreement with former semiclassical calculations for atoms and small molecules in weakly pumped cavities, while the current rigorous quantum treatment and numerical assessment sheds a light on the feasi…
The efficiency of cavity sideband cooling of trapped molecules is theoretically investigated for the case where the IR transition between two rovibrational states is used as a cycling transition. The molecules are assumed to be trapped either by a radio-frequency or optical trapping potential, depending on whether they are charged or neutral, and confined inside a high-finesse optical resonator which enhances radiative emission into the cavity mode. Using realistic experimental parameters and COS as a representative molecular example, we show that in this setup cooling to the trap ground state…
We explore whether localized surface plasmon polariton modes can transfer heat between molecules placed in the hot spot of a nanoplasmonic cavity through optomechanical interaction with the molecular vibrations. We demonstrate that external driving of the plasmon resonance indeed induces an effective molecule-molecule interaction corresponding to a new heat transfer mechanism, which can even be more effective in cooling the hotter molecule than its heating due to the vibrational pumping by the plasmon. This novel mechanism allows to actively control the rate of heat flow between molecules thro…
We propose an enantio-detection method of chiral molecules in a cavity with external drive. The chiral molecules are coupled with a quantized cavity field and two classical light fields to form the cyclic three-level systems. The chirality-dependent cavity-assisted three-photon process in the three-level systems leads to the generation of intracavity photons. Simultaneously, the drive field also results in the chirality-independent process of the generation of intracavity photons. Based on the interference between the intracavity photons generated from these two processes, one can detect the e…
Core-excitations on different atoms are highly localized and therefore decoupled. By placing molecules in an X-ray cavity the core-transitions become coupled via the exchange of cavity photons and form delocalized hybrid light-matter excitations known as core-polaritons. We demonstrate these effects for the two inequivalent carbon atoms in 1,1-difluoroethylene. Polariton signatures in the X-ray absorption, two-photon absorption, and multidimensional four-wave mixing, signals are predicted.
We consider the spontaneous emission of a broadening molecule on the surface of a micro-sphere in this paper. The density of states for the micro-cavity is derived from quasi-normal models(QNM's) expansion of the correlation functions of electromagnetic fields. Through detailed analysis we show that only weak coupling between a broadening atom(molecule) and the electromagnetic fields exists in a dielectric sphere cavity whether the sphere is small or big. From these results we find the explicit expression of the spontaneous emission decay rate for a surfactant broadening molecule on the surfac…
We theoretically investigate the phenomenon of voltage-controlled intracavity electromagnetically induced transparency with asymmetric double quantum dot system. The impact of voltage on frequency pulling and cavity linewidth narrowing are discussed. The linewidth and position of the cavity transmission can be engineered by the bias voltage. The scheme may be useful in integrated electro-optical device in quantum information process.
We study the dynamics of a supersonic molecular beam in a low-finesse optical cavity and demonstrate that most molecules in the beam can be decelerated to zero central velocity by the intracavity optical field in a process analogous to electrostatic Stark deceleration. We show that the rapid switching of the optical field for slowing the molecules is automatically generated by the cavity-induced dynamics. We further show that $\sim1\%$ of the molecules can be optically trapped at a few millikelvin in the same cavity.
We propose a mechanism to realize high-yield molecular formation from ultracold atoms. Atom pairs are continuously excited by a laser, and a collective decay into the molecular ground state is induced by a coupling to a lossy cavity mode. Using a combination of analytical and numerical techniques, we demonstrate that the molecular yield can be improved by simply increasing the number of atoms, and can overcome efficiencies of state-of-the-art association schemes. We discuss realistic experimental setups for diatomic polar and nonpolar molecules, opening up collective light matter interactions …
Two main mechanisms dictate the tunneling process in a double quantum dot: overlap of excited wave functions, effectively described as a tunneling rate, and phonon-assisted tunneling. In this paper, we study different regimes of tunneling that arise from the competition between these two mechanisms in a double quantum dot molecule immersed in a unimodal optical cavity. We show how such regimes affect the mean number of excitations in each quantum dot and in the cavity, the spectroscopic resolution and emission peaks of the photoluminescence spectrum, and the second-order coherence function whi…
We study the tunable photonic distribution in an optical molecule consisting of two linearly coupled single-mode cavities. With the inter-cavity coupling and two driving fields, the energy levels of the optical-molecule system form a closed cyclic energy-level diagram, and the phase difference between the driving fields serves as a sensitive controller on the dynamics of the system. Due to the quantum interference effect, we can realize a partially dark optical molecule, where the steady-state mean photon number in one of the cavities achieves zero even under the external driving. And the dark…
The effects caused by phonon-assisted tunnelling (PhAT) in a double quantum dot (QD) molecule immersed in a cavity were studied under the quantum Markovian master equation formalism in order to account for dissipation phenomena. We explain how for higher PhAT rates, a stronger interaction between a QD and the cavity at off-resonance takes place through the resonant interaction of another QD and the cavity, where the QDs interact through tunnelling. A closer look at the system's allowed optical transitions as a function of PhAT rates showed coalescence of the transition energies, leading to a l…
Cooling of molecules via free-space dissipative scattering of photons is thought not to be practicable due to the inherently large number of Raman loss channels available to molecules and the prohibitive expense of building multiple repumping laser systems. The use of an optical cavity to enhance coherent Rayleigh scattering into a decaying cavity mode has been suggested as a potential method to mitigate Raman loss, thereby enabling the laser cooling of molecules to ultracold temperatures. We discuss the possibility of cavity-assisted laser cooling particles without closed transitions, identif…
We propose a method for enantio-detection of chiral molecules based on a cavity-molecule system, where the left- and right-handed molecules are coupled with a cavity and two classical light fields to form cyclic three-level models. Via the cavity-assisted three-photon processes based on the cyclic three-level model, photons are generated continuously in the cavity even in the absence of external driving to the cavity. However, the photonic fields generated from the three-photon processes of left- and right-handed molecules differ with the phase difference π according to the inherent properties…
High fidelity single shot qubit state readout is essential for many quantum information processing protocols. In superconducting quantum circuit, the qubit state is usually determined by detecting the dispersive frequency shift of a microwave cavity from either transmission or reflection. In this paper, we demonstrate the use of constructive interference between the transmitted and reflected signal to optimize the qubit state readout, with which we find a better resolved state discrimination and an improved qubit readout fidelity. As a simple and convenient approach, our scheme can be combined…
We study the collective effects of an ensemble of organic molecules confined in an optical cavity based on Holstein-Tavis-Cummings model. By using the quantum Langevin approach and adiabatically eliminating the degree of freedom of the vibrational motion, we analytically obtain the expression of the cavity transmission spectrum to analyze the features of polaritonic states. As an application, we show that the dependence for the frequency shift of the lower polaritonic state on the number of molecules can be used in the detection of the ultra-cold molecules. We also numerically analyze the fluo…
In the context of the quantum-mechanical description of single-molecule surface-enhanced Raman scattering, intensity-field correlation measurements of photons emitted from a plasmonic cavity are explored, theoretically, using the technique of conditional homodyne detection. The inelastic interplay between plasmons and vibrations of a diatomic molecule placed inside the cavity can be manifested in phase-dependent third-order fluctuations of the light recorded by the aforesaid technique, allowing us to reveal signatures of non-classicality (indicatives of squeezing) of the outgoing Raman photons…
We propose a method to realize enantiodiscrimination of chiral molecules based on quantum correlation function in a driven cavity-molecule system, where the chiral molecule is coupled with a quantized cavity field and two classical light fields to form a cyclic three-level model. According to the inherent properties of electric-dipole transition moments of chiral molecules, there is a $π$-phase difference in the overall phase of the cyclic three-level model for the left- and right-handed chiral molecules. Thus, the correlation function depends on this overall phase and is chirality-dependent. …
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 propose an experimental scheme to cool and measure the three-dimensional (3D) motion of an optically trapped nanosphere in a cavity. Driven by three lasers on TEM00, TEM01, and TEM10 modes, a single cavity can cool a trapped nanosphere to the quantum ground states in all three dimensions under the resolved-sideband condition. Our scheme can also detect an individual collision between a single molecule and a cooled nanosphere efficiently. Such ability can be used to measure the mass of molecules and the surface temperature of the nanosphere. We also discuss the heating induced by the intensi…
We propose a scheme for the resonant generation of counter-polarized single photons in double asymmetric cavities with a small Kerr optical nonlinearity (as that created by a semiconductor quantum well) compared to the mode broadening. Due to the interplay between spatial intercavity tunneling and polarization coupling, by weakly exciting with circularly polarized light one of the cavities, we predict strong antibunching of counter-polarized light emission from the non-pumped auxiliary cavity. This scheme due to quantum interference is robust against surface scattering of pumping light, which …
In most theoretical descriptions of collective strong coupling of organic molecules to a cavity mode, the molecules are modeled as simple two-level systems. This picture fails to describe the rich structure provided by their internal rovibrational (nuclear) degrees of freedom. We investigate a first-principles model that fully takes into account both electronic and nuclear degrees of freedom, allowing an exploration of the phenomenon of strong coupling from an entirely new perspective. First, we demonstrate the limitations of applicability of the Born-Oppenheimer approximation in strongly coup…
Nonadiabatic phenomena are investigated in the rovibrational motion of molecules confined in an infrared cavity. Conical intersections (CIs) between vibrational polaritons, similar to CIs between electronic polaritonic surfaces, are found. The spectral, topological, and dynamic properties of the vibrational polaritons show clear fingerprints of nonadiabatic couplings between molecular vibration, rotation and the cavity photonic mode. Furthermore, it is found that for the investigated system, composed of two rovibrating HCl molecules and the cavity mode, breaking the molecular permutational sym…
Quantum Hypothesis Testing has shown the advantages that quantum resources can offer in the discrimination of competing hypothesis. Here, we apply this framework to optomechanical systems and fundamental physics questions. In particular, we focus on an optomechanical system composed of two cavities employed to perform quantum channel discrimination. We show that input squeezed optical noise, and feasible measurement schemes on the output cavity modes, allow to obtain an advantage with respect to any comparable classical schemes. We apply these results to the discrimination of models of spontan…
