Atom-photon, atom-atom and photon-photon entanglement preparation via fractional adiabatic passage

We propose a relatively robust scheme to generate maximally entangled states of (i) an atom and a cavity photon, (ii) two atoms in their ground states, and (iii) two photons in two spatially separate high-Q cavities. It is based on the interaction via fractional adiabatic passage of a three-level atom traveling through a cavity mode and a laser beam. The presence of optical phases is emphasized.

Decoherence-free creation of atom-atom entanglement in cavity via fractional adiabatic passage

We propose a robust and decoherence insensitive scheme to generate controllable entangled states of two three-level atoms interacting with an optical cavity and a laser beam. Losses due to atomic spontaneous transitions and to cavity decay are efficiently suppressed by employing fractional adiabatic passage and appropriately designed atom-field couplings. In this scheme the two atoms traverse the cavity-mode and the laser beam in opposite directions as opposed to other entanglement schemes in which the atoms are required to have fixed locations inside a cavity. We also show that the coherence of a traveling atom can be transferred to the other one without populating the cavity-mode.

Unitary time-dependent superconvergent technique for pulse-driven quantum dynamics

We present a superconvergent Kolmogorov-Arnold-Moser type of perturbation theory for time-dependent Hamiltonians. It is strictly unitary upon truncation at an arbitrary order and not restricted to periodic or quasiperiodic Hamiltonians. Moreover, for pulse-driven systems we construct explicitly the KAM transformations involved in the iterative procedure. The technique is illustrated on a two-level model perturbed by a pulsed interaction for which we obtain convergence all the way from the sudden regime to the opposite adiabatic regime.

A quantum dynamics study of the benzopyran ring opening guided by laser pulses

Abstract The ring-opening photoisomerization of benzopyran, which occurs via a photochemical route involving a conical intersection, has been studied with quantum dynamics calculations using the multi-configuration time-dependent Hartree method (MCTDH). We introduce a mechanistic strategy to control the conversion of benzopyran to merocyanine with laser pulses. We use a six-dimensional model developed in a previous work for the potential energy surfaces (PES) based on an extension of the vibronic-coupling Hamiltonian model (diabatization method by ansatz), which depends on the most active degrees of freedom. The main objective of these quantum dynamics simulations is to provide a set of str…

Fast SWAP gate by adiabatic passage

We present a process for the construction of a SWAP gate which does not require a composition of elementary gates from a universal set. We propose to employ direct techniques adapted to the preparation of this specific gate. The mechanism, based on adiabatic passage, constitutes a decoherence-free method in the sense that spontaneous emission and cavity damping are avoided.

Laser control of the radiationless decay in pyrazine using the dynamic Stark effect

The laser control of the radiationless decay between the B(3u)(nπ*) and B(2u)(ππ*) states of pyrazine using the dynamic Stark effect has been investigated. A vibronic coupling model Hamiltonian in diabatic representation, including potential energy, transition dipole, and static polarizability surfaces as a function of the four most important vibrational modes of the molecule has been parametrized using multi-reference electronic structure calculations. The interaction of the molecule with a strong non-resonant laser pulse has been analyzed in terms of dressed potential energy surfaces. Because of the large polarizability difference between the vibronically coupled B(3u)(nπ*) and B(2u)(ππ*)…

Field-free molecular alignment of asymmetric top molecules using elliptically polarized laser pulses

International audience; We show theoretically that a short specific elliptically polarized laser pulse driving an asymmetric top molecule can induce postpulse revivals of three-dimensional (3-D) alignment. By choosing the field ellipticity resulting in the best compromise between the alignment of two molecular axes, we demonstrate that efficient 3-D alignment can be achieved at low temperature. In the experiment, the field-free alignment of moderately cool ethylene molecules is probed by using a technique based on the optical Kerr effect. Control of 3-D field-free alignment opens the door to a large range of applications in chemistry as well as in molecular optics.

Propagating single photons from an open cavity: Description from universal quantization

Over the last decades, quantum optics has evolved from high quality factor cavities in the early experiments toward new cavity designs involving leaky modes. Despite very reliable models, in the concepts of cavity quantum electrodynamics, photon leakage is most of the time treated phenomenologically. Here, we take a different approach, and starting from first principles, we define an inside-outside representation which is derived from the original true-mode representation, in which one can determine effective Hamiltonian and Poynting vector. Contrary to the phenomenological model, they allow a full description of a leaking single photon produced in the cavity and propagating in free space. …

Time-dependent unitary perturbation theory for intense laser-driven molecular orientation

We apply a time-dependent perturbation theory based on unitary transformations combined with averaging techniques, on molecular orientation dynamics by ultrashort pulses. We test the validity and the accuracy of this approach on LiCl described within a rigid-rotor model and find that it is more accurate than other approximations. Furthermore, it is shown that a noticeable orientation can be achieved for experimentally standard short laser pulses of zero time average. In this case, we determine the dynamically relevant parameters by using the perturbative propagator, that is derived from this scheme, and we investigate the temperature effects on the molecular orientation dynamics.

The role of the low-lying dark np* states in the photophysics of pyrazine: a quantum dynamics study

The excited state dynamics of pyrazine has attracted considerable attention in the last three decades. It has long been recognized that after UV excitation, the dynamics of the molecule is impacted by strong non-adiabatic effects due to the existence of a conical intersection between the B2u(ππ*) and B3u(nπ*) electronic states. However, a recent study based on trajectory surface hopping dynamics simulations suggested the participation of the Au(nπ*) and B2g(nπ*) low-lying dark electronic states in the ultrafast radiationless decay of the molecule after excitation to the B2u(ππ*) state. The purpose of this work was to pursue the investigation of the role of the Au(nπ*) and B2g(nπ*) states in…

Nonintrusive monitoring and quantitative analysis of strong laser-field-induced impulsive alignment

We report the observation of impulsive alignment of $\mathrm{C}{\mathrm{O}}_{2}$ molecules produced through their interaction with a nonresonant, strong laser pulse. The periodic alignment is monitored using a polarization technique generally employed in optical Kerr effect experiments; the birefringence produced by alignment of the molecular sample is measured with a weak pulse, time-delayed with respect to the alignment pulse. The technique provides a signal proportional to $⟨{\mathrm{cos}}^{2}\phantom{\rule{0.2em}{0ex}}\ensuremath{\theta}⟩\ensuremath{-}\frac{1}{3}$, where $\ensuremath{\theta}$ is the polar angle between the molecular axis and the strong-field polarization axis. Experimen…

Generation of multiphoton Fock states by bichromatic adiabatic passage: Topological analysis

We propose a robust scheme to generate multi-photon Fock states in an atom-maser-cavity system using adiabatic passage techniques and topological properties of the dressed eigenenergy surfaces. The mechanism is an exchange of photons from the maser field into the initially empty cavity by bichromatic adiabatic passage. The number of exchanged photons depends on the design of the adiabatic dynamics through and around the conical intersections of dressed eigenenergy surfaces.

Full-dimensional control of the radiationless decay in pyrazine using the dynamic Stark effect

We present a full quantum-mechanical study of the laser control of the radiationless decay between the B3u(nπ(*)) and B2u(ππ(*)) states of pyrazine using the dynamic Stark effect. In contrast to our previous study [Sala et al., J. Chem. Phys. 140, 194309 (2014)], where a four-dimensional model was used, all the 24 degrees of freedom are now included in order to test the robustness of the strategy of control. Using a vibronic coupling Hamiltonian model in a diabatic representation, the multi-layer version of the multi-configuration time-dependent Hartree method is exploited to propagate the corresponding wave packets. We still observe a trapping of the wavepacket on the B2u(ππ(*)) potential …

Quantum averaging for driven systems with resonances

Abstract We discuss the effects of resonances in driven quantum systems within the context of quantum averaging techniques in the Floquet representation. We consider in particular iterative methods of KAM type and the extensions needed to take into account resonances. The approach consists in separating the coupling terms into resonant and nonresonant components at a given scale of time and intensity. The nonresonant part can be treated with perturbative techniques, which we formulate in terms of KAM-type unitary transformations that are close to the identity. These can be interpreted as averaging procedures with respect to the dynamics defined by effective uncoupled Hamiltonians. The reson…

Laser control for the optimal evolution of pure quantum states

Starting from an initial pure quantum state, we present a strategy for reaching a target state corresponding to the extremum (maximum or minimum) of a given observable. We show that a sequence of pulses of moderate intensity, applied at times when the average of the observable reaches its local or global extremum, constitutes a strategy transferable to different control issues. Among them, post-pulse molecular alignment and orientation are presented as examples. The robustness of such strategies with respect to experimentally relevant parameters is also examined.

Field-free one-dimensional alignment of ethylene molecule

International audience; We report an experimental study of non-adiabatic laser-induced molecular alignment of ethylene (C2H4) using a linearly polarized short laser pulse of moderate intensity. The information about the confinement of the C=C bond axis along the direction of the applied electric field is obtained by measuring the depolarization of a second short pulse of weak intensity interacting with the molecules after they have been exposed to the first pulse. The experimental data are compared with the numerical simulation of the Schr¨odinger equation written for the non-resonant interaction of an asymmetric top rigid rotor with a linearly polarized electric field. The field-free align…

Grid methods and Hilbert space basis for simulations of quantum dynamics

We discuss spatial grid methods adapted to the structure of Hilbert spaces, used to simulate quantum mechanical systems. We review the construction of Finite Basis Representation (FBR) and the Discrete Variable Representation (DVR). A mixed representation (pseudo-spectral method) is constructed through a quadrature relation linking both bases.

Topology of adiabatic passage

We examine the topology of eigenenergy surfaces characterizing the population transfer processes based on adiabatic passage. We show that this topology is the essential feature for the analysis of the population transfers and the prediction of its final result. We reinterpret diverse known processes, such as stimulated Raman adiabatic passage (STIRAP), frequency-chirped adiabatic passage and Stark-chirped rapid adiabatic passage. Moreover, using this picture, we display new related possibilities of transfer. In particular, we show that we can selectively control the level that will be populated in STIRAP process in $\ensuremath{\Lambda}$ or V systems by the choice of the peak amplitudes or …

Optimal Robust Quantum Control by Inverse Geometric Optimization

International audience; We develop an inverse geometric optimization technique that allows the derivation of optimal and robust exact solutions of low-dimension quantum control problems driven by external fields: we determine in the dynamical variable space optimal trajectories constrained to robust solutions by Euler-Lagrange optimization; the control fields are then derived from the obtained robust geodesics and the inverted dynamical equations. We apply this method, referred to as robust inverse optimization (RIO), to design optimal control fields producing a complete or half population transfer and a NOT quantum gate robust with respect to the pulse inhomogeneities. The method is versat…

Enhanced alignment and orientation of polar molecules by vibrational resonant adiabatic passage

The authors show that polar molecules can be adiabatically aligned and oriented by laser pulses more efficiently when the laser frequencies are vibrationally resonant. The aligned molecules are found in a superposition of vibrational pendular states, each associated with the alignment of the rotor in one vibrational state. The authors construct the dressed potential associated with this mechanism. Values of detunings and field amplitudes are given to optimize the degree of alignment and orientation for the CO molecule.

Adiabatic creation of entangled states by a bichromatic field designed from the topology of the dressed eigenenergies

Preparation of entangled pairs of coupled two-state systems driven by a bichromatic external field is studied. We use a system of two coupled spin-1/2 that can be translated into a three-state ladder model whose intermediate state represents the entangled state. We show that this entangled state can be prepared in a robust way with appropriate fields. Their frequencies and envelopes are derived from the topological properties of the model.

Two-laser multiphoton adiabatic passage in the frame of the Floquet theory. Applications to (1+1) and (2+1) STIRAP

We develop an adiabatic two-mode Floquet theory to analyse multiphoton coherent population transfer in N-level systems by two delayed laser pulses, which is a generalization of the three-state stimulated Raman adiabatic passage (STIRAP). The main point is that, under conditions of non-crossing and adiabaticity, the outcome and feasibility of a STIRAP process can be determined by the analysis of two features: (i) the lifting of degeneracy of dressed states at the beginning and at the end of the laser pulses, and (ii) the connectivity of these degeneracy-lifted branches in the quasienergy diagram. Both features can be determined by stationnary perturbation theory in the Floquet representation…

State-selective chirped adiabatic passage on dynamically laser-aligned molecules

We show that rovibrational state selectivity can be achieved by chirped adiabatic passage of molecules that are adiabatically aligned by a nonresonant laser field. We develop the tools to design the appropriate frequency and amplitude modulations that allow us to select a given route in the Hilbert space that leads to a final complete excitation of the chosen state, by infrared or by Raman processes. This method allows us to select a given vibrational state in a well-defined rotational $J$ state.

Orientation of Polar Molecules by Laser Induced Adiabatic Passage

International audience; We show that two overlapping linearly polarized laser pulses of frequencies ω and its second harmonic 2ω can strongly orient linear polar molecules, by adiabatic passage along dressed states. The resulting robust orientation can be interpreted as a laser-induced localization in the effective double well potential created by the fields, which induces a preliminary molecular alignment. The direction of the orientation can be selected by the relative phase of the fields.

Reaching optimally oriented molecular states by laser kicks

We present a strategy for post-pulse orientation aiming both at efficiency and maximal duration within a rotational period. We first identify the optimally oriented states which fulfill both requirements. We show that a sequence of half-cycle pulses of moderate intensity can be devised for reaching these target states.

Arbitrary qudit gates by adiabatic passage

We derive an adiabatic technique that implements the most general SU($d$) transformation in a quantum system of $d$ degenerate states, featuring a qudit. This technique is based on the factorization of the SU($d$) transformation into $d$ generalized quantum Householder reflections, each of which is implemented by a two-shot stimulated Raman adiabatic passage with appropriate static phases. The energy of the lasers needed to synthesize a single Householder reflection is shown to be remarkably constant as a function of $d$. This technique is directly applicable to a linear trapped ion system with $d+1$ ions. We implement the quantum Fourier transform numerically in a qudit with $d=4$ (defined…

Analog Grover search by adiabatic passage in a cavity-laser-atom system

A physical implementation of the adiabatic Grover search is theoretically investigated in a system of N identical three-level atoms trapped in a single mode cavity. Some of the atoms are marked through the presence of an energy gap between their two ground states. The search is controlled by two partially delayed lasers which allow a deterministic adiabatic transfer from an initially entangled state to the marked states. Pulse schemes are proposed to satisfy the Grover speedup either exactly or approximately, and the success rate of the search is calculated.

INFLUENCE OF UNEQUAL OSCILLATOR STRENGTHS ON STIMULATED RAMAN ADIABATIC PASSAGE THROUGH BRIGHT STATE

In the present work an analytical and numerical analysis of the b -STIRAP process in a medium with unequal oscillator strengths is performed. It is shown that the length of population transfer can be considerably increased by an appropriate choice of the dipole transitions.

Optimization of population transfer by adiabatic passage

We examine the adiabatic limit of population transfer in two-level models driven by a chirped laser field. We show that the nonadiabatic correction is minimized when the adiabatic eigenenergies associated to the dynamics are parallel. In the diagram of the difference of the eigenenergy surfaces as a function of the parameters, this corresponds to an adiabatic passage along a level line. The analytical arguments are based on the Dykhne-Davis-Pechukas treatment. We illustrate this behavior with various examples.

Pulse-driven near-resonant quantum adiabatic dynamics: lifting of quasi-degeneracy

We study the quantum dynamics of a two-level system driven by a pulse that starts near-resonant for small amplitudes, yielding nonadiabatic evolution, and induces an adiabatic evolution for larger amplitudes. This problem is analyzed in terms of lifting of degeneracy for rising amplitudes. It is solved exactly for the case of linear and exponential rising. Approximate solutions are given in the case of power law rising. This allows us to determine approximative formulas for the lineshape of resonant excitation by various forms of pulses such as truncated trig-pulses. We also analyze and explain the various superpositions of states that can be obtained by the Half Stark Chirped Rapid Adiabat…

Quantum dynamics by the constrained adiabatic trajectory method

We develop the constrained adiabatic trajectory method (CATM) which allows one to solve the time-dependent Schr\"odinger equation constraining the dynamics to a single Floquet eigenstate, as if it were adiabatic. This constrained Floquet state (CFS) is determined from the Hamiltonian modified by an artificial time-dependent absorbing potential whose forms are derived according to the initial conditions. The main advantage of this technique for practical implementation is that the CFS is easy to determine even for large systems since its corresponding eigenvalue is well isolated from the others through its imaginary part. The properties and limitations of the CATM are explored through simple…

Uniform analytic description of dephasing effects in two-state transitions

We describe the effect of pure dephasing upon the time-dependent dynamics of two-state quantum systems in the framework of a Lindblad equation for the time evolution of the density matrix. A uniform approximate formula is derived, which modifies the corresponding lossless transition probability by an exponential factor containing the dephasing rate and the interaction parameters. This formula is asymptotically exact in both the diabatic and adiabatic limits; comparison with numerical results shows that it is highly accurate also in the intermediate range. Several two-state models are considered in more detail, including the Landau-Zener, Rosen-Zener, Allen-Eberly, and Demkov-Kunike models, …

Field-free two-direction alignment alternation of linear molecules by elliptic laser pulses

We show that a linear molecule subjected to a short specific elliptically polarized laser field yields postpulse revivals exhibiting alignment alternatively located along the orthogonal axis and the major axis of the ellipse. The effect is experimentally demonstrated by measuring the optical Kerr effect along two different axes. The conditions ensuring an optimal field-free alternation of high alignments along both directions are derived.

Optimized time-dependent perturbation theory for pulse-driven quantum dynamics in atomic or molecular systems

We present a time-dependent perturbative approach adapted to the treatment of intense pulsed interactions. We show there is a freedom in choosing secular terms and use it to optimize the accuracy of the approximation. We apply this formulation to a unitary superconvergent technique and improve the accuracy by several orders of magnitude with respect to the Magnus expansion.

Ultrafast stimulated Raman parallel adiabatic passage by shaped pulses

We present a general and versatile technique of population transfer based on {\it parallel adiabatic passage} by femtosecond shaped pulses. Their amplitude and phase are specifically designed to optimize the adiabatic passage corresponding to parallel eigenvalues at all times. We show that this technique allows the robust adiabatic population transfer in a Raman system with the total pulse area as low as 3 $\pi$, corresponding to a fluence of one order of magnitude below the conventional stimulated Raman adiabatic passage process. This process of short duration, typically pico- and subpicosecond, is easily implementable with the modern pulse shaper technology and opens the possibility of ul…

Generation of entanglement in systems of intercoupled qubits

We consider systems of two and three qubits, mutually coupled by Heisenberg-type exchange interaction and interacting with external laser fields. We show that these systems allow one to create maximally entangled Bell states, as well as three qubit Greenberger-Horne-Zeilinger and W states. In particular, we point out that some of the target states are the eigenstates of the initial bare system. Due to this, one can create entangled states by means of pulse area and adiabatic techniques, when starting from a separable (non-entangled) ground state. On the other hand, for target states, not present initially in the eigensystem of the model, we apply the robust stimulated Raman adiabatic passag…

Control of Quantum Dynamics by Laser Pulses: Adiabatic Floquet Theory

Coherent destruction of tunneling in a six-dimensional model of NHD2: a computational study using the multi-configuration time-dependent Hartree method.

We investigate the phenomenon of coherent destruction of tunneling in a six-dimensional model of the NHD2 molecule. Two regimes are considered for the frequency of the laser field. A non-resonant regime where the frequency of the laser field is high with respect to the ground vibrational state tunneling splitting but smaller than the transition frequencies between the ground and excited vibrational states; and a quasi-resonant regime where the frequency of the laser field is close to the transition frequency between the ground and first excited vibrational states. In each case, we study the laser driven dynamics in the framework of the Floquet formalism and derive simple analytical formulas…

Effects of an environment on a cavity-quantum-electrodynamics system controlled by bichromatic adiabatic passage

International audience; We present a theoretical investigation of a cavity-QED system controlled by bichromatic adiabatic passage in a dissipative environment. We analyze the production of a controlled Fock state in the cavity by a traveling atom simultaneously coupled by a laser field, and the leakage of the corresponding photons from the cavity.

Efficient and Long-Lived Field-Free Orientation of Molecules by a Single Hybrid Short Pulse

We show that a combination of a half-cycle pulse and a short nonresonant laser pulse produces a strongly enhanced postpulse orientation. Robust transients that display both efficient and long-lived orientation are obtained. The mechanism is analyzed in terms of optimal oriented target states in finite Hilbert subspaces and shows that hybrid pulses can prove useful for other control issues.

Compact entanglement distillery using realistic quantum memories

We adopt the beam splitter model for losses to analyse the performance of a recent compact continuous-variable entanglement distillation protocol [Phys. Rev. Lett. 108, 060502, (2012)] implemented using realistic quantum memories. We show that the decoherence undergone by a two-mode squeezed state while stored in a quantum memory can strongly modify the results of the preparatory step of the protocol. We find that the well-known method for locally increasing entanglement, phonon subtraction, may not result in entanglement gain when losses are taken into account. Thus, we investigate the critical number $m_c$ of phonon subtraction attempts from the matter modes of the quantum memory. If the …

Field-free permanent molecular planar alignment

We show the existence of a permanent molecular planar alignment in field-free conditions. We present different control strategies using shaped laser pulses to reach this state. The strategies are robust with respect to the temperature and can be implemented with the state of the art technology. They can be applied not only to linear molecules but also to symmetric or asymmetric top molecules along the most polarizable molecular axis. We propose potential applications of this planar alignment such as the increase of the adsorption on a surface.

Quantum dynamics of the photostability of pyrazine

We investigate the radiationless decay of photoexcited pyrazine to its ground electronic state using multireference electronic structure and quantum dynamics calculations. We construct a quadratic vibronic coupling Hamiltonian, including the four lowest electronic states and ten vibrational modes, by fitting to more than 5000 ab initio points. We then use this model to simulate the non-adiabatic excited state dynamics of the molecule using the multi-configuration time-dependent Hartree method. On the basis of these calculations, we propose a new mechanism for this decay process involving a conical intersection between the Au(nπ*) state and the ground state. After excitation to the B2u(ππ*) …

Postpulse molecular alignment measured by a weak field polarization technique

We report a direct nonintrusive observation of alignment and planar delocalization of ${\mathrm{C}\mathrm{O}}_{2}$ after an intense linearly polarized femtosecond laser pulse excitation. The effects are measured by a polarization technique involving a perturbative probe that itself does not induce appreciable alignment. We show that this technique allows one to measure a signal proportional to $⟨{cos}^{2}\ensuremath{\theta}⟩\ensuremath{-}1/3$, with $\ensuremath{\theta}$ the angle between the molecular axis and the laser polarization. Simulations that support this analysis allow one to characterize the experimentally observed alignment and planar delocalization quantitatively.

Short-length storage of intense optical pulses in solid by adiabatic passage

We propose a novel scheme of storage of intense pulses which allows a significant reduction of the storage length with respect to standard schemes. This scheme is particularly adapted to store optical information in media with fast relaxations.

Strategies for efficient field-free molecular alignment and its control

Strategies using shaped laser fields to produce and control efficient field-free alignment are analyzed and compared. It is in particular shown that the strategy recently proposed using a shaped laser field combining an adiabatic ramp with a kick is superior to the bipulse strategy.

Implementation of single-qubit quantum gates by adiabatic passage and static laser phases

International audience; We propose and analyse experimentally feasible implementations of single-qubit quantum gates based on stimulated Raman adiabatic passage (STIRAP) between magnetic sublevels in atoms coupled by elliptically polarized pulsed laser fields, in part based on a proposal by Kis and Renzoni [Z. Kis, F. Renzoni, Phys. Rev. A 65 (2002) 032318]. These techniques require only the control of the relative phase of the driving fields but do not involve any dynamical or geometric phases, which makes it independent of the other interaction details: detuning, pulse shapes, pulse areas and pulse durations. The suggested techniques are immune to spontaneous emission since the qubit mani…

Stimulated Raman Adiabatic Passage via bright state in Lambda medium of unequal oscillator strengths

International audience; We consider the population transfer process in a Lambda-type atomic medium of unequal oscillator strengths by stimulated Raman adiabatic passage via bright-state (b-STIRAP) taking into account propagation effects. Using both analytic and numerical methods we show that the population transfer efficiency is sensitive to the ratio q(p)/q(s) of the transition oscillator strengths. We find that the case q(p) > q(s) is more detrimental for population transfer process as compared to the case where q(p) <= q(s). For this case it is possible to increase medium dimensions while permitting efficient population transfer. A criterion determining the interaction adiabaticity in th…

Pulse-driven quantum dynamics beyond the impulsive regime

We review various unitary time-dependent perturbation theories and compare them formally and numerically. We show that the Kolmogorov-Arnold-Moser technique performs better owing to both the superexponential character of correction terms and the possibility to optimize the accuracy of a given level of approximation which is explored in details here. As an illustration, we consider a two-level system driven by short pulses beyond the sudden limit.

Quantum emitter states dressed by the plasmon modes of a metal nanoparticle in the strong coupling regim

The quantum control of emitters is a key issue for quantum information processing at the nanoscale. This generally necessitates the strong coupling of emitters to a high Q-cavity for efficient manipulation of the atoms and field dynamics (cavity quantum electrodynamics or cQED). Since almost a decade, strong efforts are put to transpose cQED concepts to plasmonics in order to profit of the strong mode confinement of surface plasmons polaritons. Despite the intrinsic presence of lossy channels leading to strong decoherence in plasmonics systems, it has been experimentally proven that it is possible to reach the strong coupling regim [1].

Laser-induced enhancement of tunneling in NHD2

We apply and explore techniques aiming at enhancing the tunneling by laser fields, originally developed for a one-dimensional model, to a complete six-dimensional vibrational model of the inversion motion in NHD(2). The computational study is performed with the multi-configuration time-dependent Hartree method. Assuming an ideal three-dimensional alignment we obtain a driven tunneling time twenty times smaller than the natural one, in rather good agreement with an oversimplified three-state model. In the case of one-dimensional alignment, a linearly polarized field leads to a poor enhancement of the tunneling probability, after averaging over the rotation about the alignment axis, whereas a…

Control of field-free molecular alignment by phase-shaped laser pulses

We report an experimental study of the control of molecular alignment of ${\mathrm{N}}_{2}$ by use of spectrally modulated pulses at an intensity regime below the intrinsic saturation of the alignment. By manipulating the relative timing of the alignment revival pattern arising from the even subset of the thermal ensemble as compared to the odd subset, we demonstrate that the angular distribution of the aligned molecule can be converted into planar delocalization at specific times. We also show that the angular focusing of the molecular axis can be switched off by applying a specific bipulse.

Optimized adiabatic passage with dephasing

We study adiabatic population transfer with dephasing in two-level models driven by a chirped driving field. We show that the population transfer is maximized when the dynamics follows specific ellipses as trajectories in the parameter space. We determine the optimal parameters and estimate the losses in a closed form. These estimates show a similar robustness as for the standard lossless adiabatic processes with respect to variations of the parameters.

Field-free molecular alignment induced by elliptically polarized laser pulses: Noninvasive three-dimensional characterization

International audience; An investigation of field-free molecular alignment produced by elliptically polarized laser pulses is reported. Experiments are conducted in CO2 at room temperature. A noninvasive all-optical technique, based on the cross defocusing of a probe pulse, is used to measure the alignment along two orthogonal directions which is sufficient to provide a three-dimensional characterization. The field-free molecular alignment produced by a laser of elliptical polarization is in good agreement in terms of amplitude and shape with theoretical predictions. It turns out to be almost equivalent to the superposition of the effects that one would obtain with two individual cross-pola…

Theory of the bright-state stimulated Raman adiabatic passage

We describe analytically and numerically the process of population transfer by stimulated Raman adiabatic passage through a bright state when the pulses propagate in a medium. Limitations of the adiabaticity are analyzed and interpreted in terms of reshaping of the pulses. We find parameters for the pulses for which the population transfer is nearly complete over long distances.

Optical gratings induced by field-free alignment of molecules

We analyze the alignment of molecules generated by a pair of crossed ultra-short pump pulses of different polarizations by a technique based on the induced time-dependent gratings. Parallel polarizations yield an intensity grating, while perpendicular polarizations induce a polarization grating. We show that both configurations can be interpreted at moderate intensity as an alignment induced by a single polarized pump pulse. The advantage of the perpendicular polarizations is to give a signal of alignment that is free from the plasma contribution. Experiments on femtosecond transient gratings with aligned molecules were performed in CO2 at room temperature in a static cell and at 30 K in a …

Optimization of field-free molecular alignment by phase-shaped laser pulses

We theoretically demonstrate the optimization of field-free molecular alignment by phase-shaped femtosecond laser pulses. The effect is assessed in ${\mathrm{O}}_{2}$ at $T=60\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ under realistic conditions of intensity and pulse shaping. The spectral laser phase is sampled through 128 control parameters and a self-learning evolutionary algorithm combined with a nonperturbative regime calculation is used in order to design the specific phase that maximizes the degree of alignment. The postpulse molecular alignment appears significantly enhanced compared to a Fourier-transform-limited pulse of same energy. The analysis of the target state reveals that the so…

Adiabatic evolution for systems with infinitely many eigenvalue crossings

International audience; We formulate an adiabatic theorem adapted to models that present an instantaneous eigenvalue experiencing an infinite number of crossings with the rest of the spectrum. We give an upper bound on the leading correction terms with respect to the adiabatic limit. The result requires only differentiability of the considered projector, and some geometric hypothesis on the local behavior of the eigenvalues at the crossings.

Quantum search by parallel eigenvalue adiabatic passage

We propose a strategy to achieve the Grover search algorithm by adiabatic passage in a very efficient way. An adiabatic process can be characterized by the instantaneous eigenvalues of the pertaining Hamiltonian, some of which form a gap. The key to the efficiency is based on the use of parallel eigenvalues. This allows us to obtain non-adiabatic losses which are exponentially small, independently of the number of items in the database in which the search is performed.

Quantum plasmonics with multi-emitters: application to stimulated Raman adiabatic passage

We construct a mode-selective effective model describing the interaction of the localised surface plasmon polaritons (LSPs) supported by a spherical metal nanoparticle (MNP) with N quantum emitters (QEs) in an arbitrary geometric arrangement. Simplifying previously presented procedures, we develop a formulation in which the field response in the presence of the MNP can be decomposed into orthogonal modes, expanding the Green tensor of the system in the spherical vector harmonics basis and using the generalized global Löwdin orthogonalization algorithm. We investigate the possibility of using the LSPs as mediators of an efficient control of population transfer between two QEs. We show that a…

Eigenfunction expansions for time dependent hamiltonians

We describe a generalization of Floquet theory for non periodic time dependent Hamiltonians. It allows to express the time evolution in terms of an expansion in eigenfunctions of a generalized quasienergy operator. We discuss a conjecture on the extension of the adiabatic theorem to this type of systems, which gives a procedure for the physical preparation of Floquet states. *** DIRECT SUPPORT *** A3418380 00004

Optimal adiabatic passage by shaped pulses: Efficiency and robustness

We explore the efficiency and robustness of population transfer in two-state systems by adiabatic passage (i) when the driving pulse is optimally designed in order to lead to parallel adiabatic passage or (ii) with a linear chirping. We show how one could practically implement the corresponding designs of the pulses in the spectral domain. We analyze the robustness of the two shapings taking into account fluctuations of the phase, amplitude, and the area of the pulse. We show the overall superiority of the parallel adiabatic passage especially when one faces the issue of a pulse area that is not well known. We show that the robustness of parallel adiabatic passage is not improved when it is…

Adiabatic approximation for quantum dissipative systems: formulation, topology and superadiabatic tracking

A generalized adiabatic approximation is formulated for a two-state dissipative Hamiltonian which is valid beyond weak dissipation regimes. The history of the adiabatic passage is described by superadiabatic bases as in the nondissipative regime. The topology of the eigenvalue surfaces shows that the population transfer requires, in general, a strong coupling with respect to the dissipation rate. We present, furthermore, an extension of the Davis-Dykhne-Pechukas formula to the dissipative regime using the formalism of Stokes lines. Processes of population transfer by an external frequency-chirped pulse-shaped field are given as examples.

Ultimate field-free molecular alignment by combined adiabatic-impulsive field design

We show that a laser pulse designed as an adiabatic ramp followed by a kick allows one to reach a perfect postpulse molecular alignment, free of saturation. The mechanism is based on an optimized distribution of the energy between a weakly efficient but non saturating adiabatic ramp and an efficient but saturating impulsive field. Unprecedent degrees of alignment are predicted using state-of-the-art pulse shaping techniques and non-destructive field intensities. The scheme can be extended to reach high degrees of orientation of polar molecules using designed half-cycle pulses.

Suppression of plasma contribution in femtosecond degenerate four-wave mixing (fs-DFWM) at high intensity

Femtosecond degenerate four-wave mixing (fs-DFWM) experiments in CO2 exhibit a strong background due to plasma produced at high intensity (≥20 TW/cm2), when significant molecular alignment is likely to arise. This perturbing phenomenon renders the measurements of alignment very difficult. It is shown that the plasma contribution can be avoided by employing perpendicular polarizations for the two pump pulses. The effect is explained on the basis of the different diffraction angles between signals produced by molecular alignment and plasma. Copyright © 2007 John Wiley & Sons, Ltd.

Quantum state engineering in a cavity by Stark chirped rapid adiabatic passage

We propose a robust scheme to generate single-photon Fock states and atom-photon and atom-atom entanglement in atom-cavity systems. We also present a scheme for quantum networking between two cavity nodes using an atomic channel. The mechanism is based on Stark-chirped rapid adiabatic passage (SCRAP) and half-SCRAP processes in a microwave cavity. The engineering of these states depends on the design of the adiabatic dynamics through the static and dynamic Stark shifts.

Arbitrary state controlled-unitary gate by adiabatic passage

We propose a robust scheme involving atoms fixed in an optical cavity to directly implement the universal controlled-unitary gate. The present technique based on adiabatic passage uses novel dark states well suited for the controlled-rotation operation. We show that these dark states allow the robust implementation of a gate that is a generalisation of the controlled-unitary gate to the case where the control qubit can be selected to be an arbitrary state. This gate has potential applications to the rapid implementation of quantum algorithms such as of the projective measurement algorithm. This process is decoherence-free since excited atomic states and cavity modes are not populated during…

Robust control of unstable nonlinear quantum systems

Adiabatic passage is a standard tool for achieving robust transfer in quantum systems. We show that, in the context of driven nonlinear Hamiltonian systems, adiabatic passage becomes highly non-robust when the target is unstable. We show this result for a generic (1:2) resonance, for which the complete transfer corresponds to a hyperbolic fixed point in the classical phase space featuring an adiabatic connectivity strongly sensitive to small perturbations of the model. By inverse engineering, we devise high-fidelity and robust partially non-adiabatic trajectories. They localize at the approach of the target near the stable manifold of the separatrix, which drives the dynamics towards the ta…

Adiabatic quantum search scheme with atoms in a cavity driven by lasers

We propose an implementation of the quantum search algorithm of a marked item in an unsorted list of N items by adiabatic passage in a cavity-laser-atom system. We use an ensemble of N identical three-level atoms trapped in a single-mode cavity and driven by two lasers. In each atom, the same level represents a database entry. One of the atoms is marked by having an energy gap between its two ground states. Appropriate time delays between the two laser pulses allow one to populate the marked state starting from an initial entangled state within a decoherence-free adiabatic subspace. The time to achieve such a process is shown to exhibit the Grover speedup.

Robust quantum control by a single-shot shaped pulse

Considering the problem of the control of a two-state quantum system by an external field, we establish a general and versatile method allowing the derivation of smooth pulses which feature the properties of high fidelity, robustness, and low area. Such shaped pulses can be interpreted as a single-shot generalization of the composite pulse-sequence technique with a time-dependent phase.

Control of Localization and Suppression of Tunneling by Adiabatic Passage

We show that a field of frequency $\ensuremath{\omega}$ combined with its second harmonic $2\ensuremath{\omega}$ driving a double-well potential allows us to localize the wave packet by adiabatic passage, starting from the delocalized ground state. The relative phase of the fields allows us to choose the well of localization. We can suppress (and restore) the tunneling subsequently by switching on (and off) abruptly the fields at well-defined times. The mechanism relies on the fact that the dynamics is driven to an eigenstate of the Floquet Hamiltonian which is a localized state.

Preparation of coherent superposition in a three-state system by adiabatic passage

We examine the topology of eigenenergy surfaces associated to a three-state system driven by two quasi-resonant fields. We deduce mechanisms that allow us to generate various coherent superposition of two states using an additional field, far off resonances. We report the numerical validations in mercury atoms as a model system, creating the coherent superpositions of two excited states and of two states coupled by a Raman process.

Bichromatic field propagation in a resonant medium: Floquet analysis

We study the propagation of a bichromatic field in a resonant medium. The two modes of the incoming fields are pulsed and delayed with respect to each other. It is shown that in the course of the propagation, new Raman sidebands will be generated. The achievable frequency spacing between the sidebands is determined from experimental data. A numerical example is shown for realistic physical parameters.

Dressed states of a quantum emitter strongly coupled to a metal nanoparticle

Hybrid molecule-plasmonic nanostructures have demonstrated their potential for surface enhanced spectroscopies, sensing, or quantum control at the nanoscale. In this Letter, we investigate the strong coupling regime and explicitly describe the hybridization between the localized plasmons of a metal nanoparticle and the excited state of a quantum emitter, offering a simple and precise understanding of the energy exchange in full analogy with cavity quantum electrodynamics treatment and a dressed atom picture. Both near-field emission and far-field radiation are discussed, revealing the richness of such optical nanosources.

Floquet perturbative analysis for STIRAP beyond the rotating wave approximation

We present a perturbative analysis of Floquet eigenstates in the context of two delayed laser processes (STIRAP) in three level systems. We show the efficiency of a systematic perturbative development which can be applied as long as no non-linear resonances occur.

Efficient adiabatic tracking of driven quantum nonlinear systems

We derive a technique of robust and efficient adiabatic passage for a driven nonlinear quantum system, describing the transfer to a molecular Bose-Einstein condensate from an atomic one by external fields. The pulse ingredients are obtained by tracking the dynamics derived from a Hamiltonian formulation, in the adiabatic limit. This leads to a nonsymmetric and nonmonotonic chirp. The efficiency of the method is demonstrated in terms of classical phase space, more specifically with the underlying fixed points and separatrices. We also prove the crucial property that this nonlinear system does not have any solution leading exactly to a complete transfer. It can only be reached asymptotically …

Fast and robust population transfer in two-level quantum systems with dephasing noise and/or systematic frequency errors

We design, by invariant-based inverse engineering, driving fields that invert the population of a two-level atom in a given time, robustly with respect to dephasing noise and/or systematic frequency shifts. Without imposing constraints, optimal protocols are insensitive to the perturbations but need an infinite energy. For a constrained value of the Rabi frequency, a flat $\pi$ pulse is the least sensitive protocol to phase noise but not to systematic frequency shifts, for which we describe and optimize a family of protocols.

Quantum logic gates by adiabatic passage

International audience; We present adiabatic passage techniques for the realisation of one and two-qubit quantum Gates. These methods use evolution along dark-states of the system, avoiding decoherence effects such as spontaneous emission. The advantage of these methods is their robustness: they are insensitive to the fluctuations of the parameters and to partial knowledge of the system.