Microcavities have been shown to influence the reactivity of molecular ensembles by strong coupling of molecular vibrations to quantized cavity modes. In quantum mechanical treatments of such scenarios, frequently idealized models with single molecules and scaled, effective molecule-cavity interactions or alternatively ensemble models with simplified model Hamiltonians are used. In this work, we go beyond these models by applying an ensemble variant of the Pauli-Fierz Hamiltonian for vibro-polaritonic chemistry and numerically solve the underlying time-dependent Schrödinger equation to study the cavity-induced quantum dynamics in an ensemble of thioacetylacetone (TAA) molecules undergoing hydrogen transfer under vibrational strong coupling (VSC) conditions. Beginning with a single molecule coupled to a single cavity mode, we show that the cavity indeed enforces hydrogen transfer from an enol to an enethiol configuration with transfer rates significantly increasing with light-matter interaction strength. This positive effect of the cavity on reaction rates is different from several other systems studied so far, where a retarding effect of the cavity on rates was found. It is argued that the cavity ``catalyzes'' the reaction by transfer of virtual photons to the molecule. The same concept applies to ensembles with up to $N=20$ TAA molecules coupled to a single cavity mode, where an additional, significant, ensemble-induced collective isomerization rate enhancement is found. The latter is traced back to complex entanglement dynamics of the ensemble, which we quantify by means of von Neumann-entropies. A non-trivial dependence of the dynamics on ensemble size is found, clearly beyond scaled single-molecule models, which we interpret as transition from a multi-mode Rabi to a system-bath-type regime as $N$ increases.
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 …
We analytically obtain the maximum probability of converting a finite number of copies of an arbitrary two-qubit pure state to a single copy of a maximally entangled two-qubit pure state via entanglement assisted local operations and classical communications using a two-qubit catalyst state. We show that the optimal catalyst for this transformation is always more entangled than the initial state but any two-qubit state can act as a (non-optimal) catalyst. Interestingly, the entanglement of the optimal two-qubit catalyst state is shown to decrease with that of the initial state. Entanglement as…
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 propose a scheme for preparation of entangled coherent states for the motion of an ion in a two-dimensional anisotropic trap. In the scheme, the ion is driven by four laser beams along different directions in the ion trap plane, resulting in carrier excitation and couplings between the internal and external degrees of freedom. When the total quantum number of the vibrational modes initially has a definite parity, the competition between the unitary dynamics and spontaneous emission will force the system to evolve to a steady state, where the vibrational modes are in a two-mode cat state. We…
Probing high-frequency gravitational waves with entangled vibrational qubits in linear Paul traps
KEK Theory Center（高能加速器研究机构理论中心）；The Graduate University for Advanced Studies, SOKENDAI（高级研究大学院大学（SOKENDAI））；Yukawa Institute for Theoretical Physics, Kyoto University（京都大学汤川理论物理研究所）
We show how entangled qubits can be encoded as entangled coherent states of two-dimensional centre-of-mass vibrational motion for two ions in an ion trap. The entangled qubit state is equivalent to the canonical Bell state, and we introduce a proposal for entanglement transfer from the two vibrational modes to the electronic states of the two ions in order for the Bell state to be detected by resonance fluorescence shelving methods.
We propose an ideal scheme for preparing vibrational $\mathrm{SU(1,1)} \otimes \mathrm{SU(1,1)}$ states in a two-dimensional ion trap using red and blue second sideband resolved driving of two orthogonal vibrational modes. Symmetric and asymmetric driving provide two regimes to realize quantum state engineering of the vibrational modes. In one regime, we show that time evolution synthesizes so-called $\mathrm{SU}(1,1)$ Perelomov coherent states, that is separable squeezed states and their superposition too. The other regime allows engineering of lossless 50/50 $\mathrm{SU}(2)$ beam splitter st…
Macroscopic entangled cat states not only are significant in the demonstration of the fundamentals of quantum physics, but also have wide applications in modern quantum technologies such as continuous-variable quantum information processing and quantum metrology. Here we propose a scheme for generation of macroscopic entangled cat states in a molecular cavity-QED system, which is composed of an organic molecule (including electronic and vibrational states) coupled to a single-mode cavity field. By simultaneously modulating the resonance frequencies of the molecular vibration and the cavity fie…
We consider a trapped ion with a quantized center-of-mass motion in 2D trap potential. With external laser fields the effective (non)linear coupling of two orthogonal vibrational modes can be established via stimulated Raman transition. Nonclassical vibrational states such as squeezed states or two-mode entangled states (Schroedinger cat-like states) can be generated. When the vibrational modes are entangled with internal energy levels the Greenberger-Horne-Zeilinger (GHZ) states can be prepared.
In this work, we provided a proof-of-principle of efficient production of maximally entangled states using charged quantum dots coupled to vibrational modes. The physical system consists of two pairs of quantum dots, each pair with a single electron able to tunnel between the dots, thus encoding a qubit. The electrons, initially not coupled, interact with two bosonic vibrational modes. It is demonstrated that the electron-vibrational mode coupling drives to an effective electron-electron interaction, which is the main mechanism behind the formation of maximally quantum entangled electronic sta…
We apply estimation theory to a system formed by two interacting trapped ions. By using the Fisher matrix formalism, we introduce a simple scheme for estimation of the temperature of the longitudinal vibrational modes of the ions. We use the ions interaction to effectively infer the temperature of the individual ions, by optimising the interaction time evolution and by measuring only over one of the ions. We also investigate the effect of a non-thermal reservoir over the inference approach. The non-classicality of one of the ions vibrational modes, introduced due to a squeezed thermal reservoi…
A compact scheme for the preparation of macroscopic multipartite entanglement is proposed and analyzed. In this scheme the vibrational modes of a mechanical resonator constitute continuous variable (CV) subsystems that entangle to each other as a result of their interaction with a two-level system (TLS). By properly driving the TLS, we show that a selected set of modes can be activated and prepared in a multipartite entangled state. We first study entanglement properties of a three-mode system by evaluating the genuine multipartite entanglement. And investigate its usefulness as a quantum reso…
We present a universal algorithm for an efficient deterministic preparation of an arbitrary two--mode bosonic state. In particular, we discuss in detail preparation of entangled states of a two-dimensional vibrational motion of a trapped ion via a sequence of laser stimulated Raman transitions. Our formalism can be generalized for multi-mode bosonic fields. We examine stability of our algorithm with respect to a technical noise.
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 …
Effects of non-linear coupling between the system and the bath vibrational modes on the system internal conversion dynamics are investigated using the Dirac-Frenkel variational approach with the defined sD2 ansatz. It explicitly accounts for the entangled system electron-vibrational wavepacket states, while the bath quantum harmonic oscillator (QHO) states are expanded in a superposition of coherent states (CS). Using a non-adiabatically coupled three-level model, we show that quadratic system-bath coupling induces non-reversible internal conversion when the bath QHO wavepacket representation …
We present an efficient scheme to generate two-mode SU(2) macroscopic quantum superposition (Schrödinger cat) states, entangled number states and entangled coherent states for the vibrational motion of an ion trapped in a two-dimensional harmonic potential well. We also show that the same scheme can be used to realize a Fredkin gate operation.
We develop an ultrafast frequency-resolved Raman spectroscopy with entangled photons for polyatomic molecules in condensed phases, to probe the electronic and vibrational coherences. Using quantum correlation between the photons, the signal shows the capability of both temporal and spectral resolutions that are not accessible by either classical pulses or the fields without entanglement. We develop a microscopic theory for this Raman spectroscopy, revealing the electronic coherence dynamics which often shows a rapid decay within $\sim$50fs. The heterodyne-detected Raman signal is further devel…
Analytical solution of the Schrodinger equation for the neutral helium atom in the ground state considering the uncertainty principle, vibrational modes and quantum-electrodynamical effects
The quantum photodynamics of a simple diatomic molecule with a permanent dipole immersed within an optical cavity containing a quantized radiation field is studied in detail. The chosen molecule under study, lithium fluoride (LiF), is characterized by the presence of an avoided crossing between the two lowest $^1Σ$ potential energy curves (covalent-ionic diabatic crossing). Without field, after prompt excitation from the ground state $1\; ^1Σ$, the excited nuclear wave packet moves back and forth in the upper $2\; ^1Σ$ state, but in the proximity of the avoided crossing, the non-adiabatic coup…
We develop the analytic theory describing the formation and evolution of entangled quantum states for a fermionic quantum emitter coupled to a quantized electromagnetic field in a nanocavity and quantized phonon or mechanical vibrational modes. The theory is applicable to a broad range of cavity quantum optomechanics problems and emerging research on plasmonic nanocavities coupled to single molecules and other quantum emitters. The optimal conditions for a tri-state entanglement are realized near the parametric resonances in a coupled system. The model includes decoherence effects due to coupl…
Simulating Electron Transfer on Noisy Quantum Computers
Institute of Engineering Thermodynamics, German Aerospace Center (DLR)（德国航空航天中心工程热力学研究所）；Helmholtz Institute Ulm（乌尔姆亥姆霍兹研究所）；Institute of Software Technology, German Aerospace Center (DLR)（德国航空航天中心软件技术研究所）；HQS Quantum Simulations GmbH（HQS量子模拟有限公司）；Department of Physics, Ulm University（乌尔姆大学物理系）
I propose an efficient method for measuring non-linear coupling between the collective axial breathing mode and the radial rocking mode induced by the mutual Coulomb repulsion in linear ion crystal. The quantum sensing technique is based on the laser induced coupling between one of the vibrational modes and the internal ion's spin states which allows to estimate the non-linear coupling either by measuring the phonon probability distribution or directly be observing the Ramsey-type oscillations of the ion spin states. I show that due to the presence of non-linear phonon coupling the off-resonan…
We analyze the dynamics of a chain of singly-charged ions confined in a linear Paul trap and which couple with the mode of a high-finesse optical resonator. In these settings the ions interact via the Coulomb repulsion and are subject to the mechanical forces due to scattering of cavity photons. We show that the interplay of these interactions can give rise to bistable equilibrium configurations, into which the chain can be cooled by cavity-enhanced photon scattering. We characterize the resulting equilibrium structures by determining the stationary state in the semiclassical limit for both ca…
Here we present a fundamental study on how the ground-state chemical reactivity of a molecule can be modified in a QED scenario, i.e., when it is placed inside a cavity and there is strong coupling between the cavity field and vibrational modes within the molecule. We work with a model system for the molecule (Shin-Metiu model) in which nuclear, electronic and photonic degrees of freedom are treated on the same footing. This simplified model allows the comparison of exact quantum reaction rate calculations with predictions emerging from transition state theory based on the cavity Born-Oppenhei…
Entanglement of bosonic modes of material oscillators is studied in the context of two bilinearly coupled, nonlinear oscillators. These oscillators are realizable in the vibrational-cum-bending motions of C-H bonds in dihalomethanes. The bilinear coupling gives rise to invariant subspaces in the Hilbert space of the two oscillators. The number of separable states in any invariant subspace is one more than the dimension of the space. The dynamics of the oscillators when the initial state belongs to an invariant subspace is studied. In particular, the dynamics of the system when the initial stat…
Single Spatio-Temporal Mode Bright Twin-Beam Source Across the Near- and Mid-Infrared
Polytechnique Montréal（蒙特利尔理工学院）；Universidad Del Valle（德瓦列大学）；Institut Interdisciplinaire d’Innovation Technologique, Université de Sherbrooke（舍布鲁克大学跨学科技术创新研究所）；Max Planck Institute for the Science of Light（马克斯·普朗克光科学研究所）；Friedrich-Alexander-Universität Erlangen-Nürnberg (FAU)（埃尔朗根-纽伦堡弗里德里希·亚历山大大学）
