Coherent Population Transfer Research Articles

Coherent trapping in small quantum networks

We consider a three-node fully connected network (Delta network) showing that a coherent population trapping phenomenon occurs, generalizing results for the Lambda network known to support a dark state. Transport in such structures provides signatures of detrapping, which can be triggered by external controls. In the presence of an environment it turns out to be sensitive to its Markovianity. Adiabatic modulation of the system’s parameters may yield coherent population transfer, analogous to the stimulated Raman adiabatic passage phenomenon. Robustness of this protocol against non-adiabatic transitions is studied. Coherent nanostructures where these phenomena are relevant for quantum transport and quantum protocols are suggested.

Rotational, Vibrational, and Electronic Modulations in N_{2}^{+} Lasing at 391nm: Evidence of Coherent B^{2}Σ_{u}^{+}-X^{2}Σ_{g}^{+}-A^{2}Π_{u} Coupling.

We investigate lasing of a N_{2} gas induced by intense few-cycle near-IR laser pulses. By the pump-probe measurements, we reveal that the intensity of the B^{2}Σ_{u}^{+}-X^{2}Σ_{g}^{+} lasing emission of N_{2}^{+} oscillates at high (0.3-0.5PHz), medium (50-75THz), and low (∼3 THz) frequencies, corresponding to the energy separations between the rovibrational levels of the A^{2}Π_{u} and X^{2}Σ_{g}^{+} states. By solving the time-dependent Schrödinger equation, we reproduce the oscillations in the three different frequency ranges and show that the coherent population transfer among the three electronic states of N_{2}^{+} creates the population inversion between the B^{2}Σ_{u}^{+} and X^{2}Σ_{g}^{+} states, resulting in the lasing at 391nm.

Improving coherent population transfer via a stricter adiabatic condition

High-fidelity and robust coherent population transfer is a major challenge in coherent quantum control. Different from the well known adiabatic condition, we present a rigorous adiabatic condition that is inspired by the idea of the Landau-Zener tunneling. Based on this, we propose a coherent population transfer approach, which just needs only one control parameter and depends on the eigenvalues of the systems. Compared to other approaches, such as fast quasiadiabatic dynamics, shortcut to adiabatic passage, we numerically demonstrate that our approach can provide a more high-fidelity and more robustness coherent population transfer without affecting the speed. In short, our approach opens a new way to further increase the fidelity and the robustness of coherent population transfer. Moreover, it may be generalized to complex quantum systems where the exact expressions of eigenstates are difficult to obtain or the paremeters of systems are difficult to simultaneously drive.

Ultrastrong coupling probed by Coherent Population Transfer

Light-matter interaction, and the understanding of the fundamental physics behind, is the scenario of emerging quantum technologies. Solid state devices allow the exploration of new regimes where ultrastrong coupling strengths are comparable to subsystem energies, and new exotic phenomena like quantum phase transitions and ground-state entanglement occur. While experiments so far provided only spectroscopic evidence of ultrastrong coupling, we propose a new dynamical protocol for detecting virtual photon pairs in the dressed eigenstates. This is the fingerprint of the violated conservation of the number of excitations, which heralds the symmetry broken by ultrastrong coupling. We show that in flux-based superconducting architectures this photon production channel can be coherently amplified by Stimulated Raman Adiabatic Passage, providing a unique tool for an unambiguous dynamical detection of ultrastrong coupling in present day hardware. This protocol could be a benchmark for control of the dynamics of ultrastrong coupling architectures, in view of applications to quantum information and microwave quantum photonics.

Selective excitation of vibrational modes and probe for asymmetric intramolecular energy redistribution

Femtosecond time- and frequency-resolved coherent anti-Stokes Raman scattering spectroscopy was performed on liquid nitrobenzene (NB) to explore intramolecular vibrational energy redistribution in the electronic ground state. While high-frequency C–H stretching vibrational modes (vCH ∼ 3080 cm−1) were selectively excited, vibrational energy redistribution to the nitro group and phenyl ring breathing modes ( ∼ 1335 cm−1, ∼ 1514 cm−1 and ∼1584 cm−1) was described. While lower frequency modes of the nitro group and phenyl ring breathing were selectively excited, vibrational energy redistribution to C–H stretching modes with higher efficiency was detected. There is counter-intuitive vibrational energy flow in NB. Vibrational energy redistribution was discussed in the view of coherent population transfer between parent modes. Coherent coupling of these relevant modes and the selectivity of vibrational energy redistribution were further analyzed from the viewpoint of vibrational symmetry.

Translational cooling of doped nanocrystals by Raman pulses: Towards macroscopic quantum state

One of the most interesting problems of modern physics is the realization of nanoparticles in macroscopic quantum states, in which they behave as a quantum objects. These states can only be implemented at ultra-low translational temperatures that have not been achieved so far. Here we develop a novel method for optical cooling of CaF2:Yb3+ nanocrystals, which is based on the coherent population transfer induced in the impurity ions by ultraviolet Raman pulses. A doped nanocrystal localized in a radio-frequency trap is cooled due to the photon recoil from the pulses of varied intensity. The proposed method allows to obtain nanocrystals with translational temperatures of the order of 10−9 K, which indicates that the nanocrystal approaches a macroscopic quantum state.

State-Specific Enrichment of Chiral Conformers with Microwave Spectroscopy.

An interesting class of molecules is that in which the molecules do not possess a stereogenic center but can become chiral because of their spatial arrangement. These molecules can be seen as chiral conformers, whose two nonsuperimposable forms can interconvert from one to another by rotations about single bonds. Here, we show that an initially racemic mixture of chiral conformers, such as a sample of cyclohexylmethanol, C7H14O, can be enantiomerically enriched by performing the enantioselective process of coherent population transfer between rotational levels. By first performing a population transfer cycle, followed by a three-wave mixing experiment, we show that an enantiomeric excess in a rotational level of choice can be achieved. This represents the first experimental demonstration of such an effect in a chiral pair of conformers, and it showcases the broad applicability of three-wave mixing not only for analytical applications but also to a wide scope of experiments of fundamental interest.

Coherent population transfer with Laguerre–Gaussian pulses

We report a scheme to achieve coherent population transfer in a four-level double- closed-loop atomic system by utilizing the coherent beams with Laguerre–Gaussian profiles. It is demonstrated that a maximal population transfer is achieved for a special value of the relative phase of the applied fields. We then compare the results with a similar configuration, but for the laser pulses with the usual Gaussian profiles and conclude that using the Laguerre–Gaussian modes can result in almost complete population transfer. Besides, the creation of a superposition between two lower states can be achieved through properly changing the relative phase. The suggested scheme may hold great practicality for the realization of the population transfer as well as creation of the superposition between states in the quantum systems with multiple states.

Tracking coherent population transfer and thermal population relaxation in condensed system by broad-band transient grating spectroscopy

Broad-band transient grating (BB-TG) spectroscopy was proposed to track both coherent population transfer (CPT) and thermal population relaxation processes in a condensed system of solvated molecules in solution (Rhodamine101 in methanol). A broad band around 1500 cm−1 and a relative narrow band near 2900 cm−1 emerge in TG and transient absorption contour plots when pump and probe pulses overlap in the sample. The experimental results matched well with the vibrational modes of Rhodamine101 that were obtained by theoretical calculation. In addition, it was found that the population of CPT particles can be evaluated quantitatively through the intensity of the TG signal.

Coherent population transfer in multi-level Allen–Eberly models

We investigate the solvability of multi-level extensions of the Allen–Eberly model and the population transfer yielded by the corresponding dynamical evolution. We demonstrate that, under a matching condition of the frequency, the driven two-level system and its multi-level extensions possess a stationary-state solution in a canonical representation associated with a unitary transformation. As a consequence, we show that the resulting protocol is able to realize complete population transfer in a nonadiabatic manner. Moreover, we explore the imperfect pulsing process with truncation and display that the nonadiabatic effect in the evolution can lead to suppression to the cutoff error of the protocol.

Coherent laser-millimeter-wave interactions en route to coherent population transfer.

We demonstrate coherent two-photon population transfer to Rydberg states of barium atoms using a combination of a pulsed dye laser and a chirped-pulse millimeter-wave spectrometer. Numerical calculations, using a density matrix formalism, reproduce our experimental results and explain the factors responsible for the observed fractional population transferred, optimal experimental conditions, and possibilities for future improvements. The long coherence times associated with the millimeter-wave radiation aid in creating coherence between the ground state and Rydberg states, but higher-coherence laser sources are required to achieve stimulated Raman adiabatic passage and for applications to molecules.

Measuring the polarization of electromagnetic fields using Rabi-rate measurements with spatial resolution: Experiment and theory

When internal states of atoms are manipulated using coherent optical or radio-frequency (RF) radiation, it is essential to know the polarization of the radiation with respect to the quantization axis of the atom. We first present a measurement of the two-dimensional spatial distribution of the electric-field amplitude of a linearly-polarized pulsed RF electric field at $\sim 25.6\,$GHz and its angle with respect to a static electric field. The measurements exploit coherent population transfer between the $35$s and $35$p Rydberg states of helium atoms in a pulsed supersonic beam. Based on this experimental result, we develop a general framework in the form of a set of equations relating the five independent polarization parameters of a coherently oscillating field in a fixed laboratory frame to Rabi rates of transitions between a ground and three excited states of an atom with arbitrary quantization axis. We then explain how these equations can be used to fully characterize the polarization in a minimum of five Rabi rate measurements by rotation of an external bias-field, or, knowing the polarization of the driving field, to determine the orientation of the static field using two measurements. The presented technique is not limited to Rydberg atoms and RF fields but can also be applied to characterize optical fields. The technique has potential for sensing the spatiotemporal properties of electromagnetic fields, e.g., in metrology devices or in hybrid experiments involving atoms close to surfaces.

Enantiomer-Specific State Transfer of Chiral Molecules

State-selective enantiomeric excess is realized using microwave-driven coherent population transfer. The method selectively promotes either R or S molecules to a higher rotational state by phase-controlled microwave pulses that drive electric-dipole allowed rotational transitions. We demonstrate the enantiomer-specific state transfer method using enantiopure samples of 1,2-propanediol. This method of state-specific enantiomeric enrichment can be applied to a large class of asymmetric, chiral molecules that can be vaporized and cooled to the point where rotationally resolved spectroscopy is possible, including molecules that rapidly racemize. The rapid chiral switching demonstrated here allows for new approaches in high-precision spectroscopic searches for parity violation in chiral molecules.

Strong coupling and ultrafast dynamics in organic semiconductor/metal hybrid nanostructures

Active plasmonics, as an important branch of Plasmonics, is growing rapidly over the last decades. The main principle of active plasmonics is to combine surface plasmon polaritons (SPPs) with ‘active’ materials to com-penstate intrinsic weak optical nonlinearities and short propagation lengths of SPPs, so that external manipula-tion and coherent control of SPPs can be realized. Here, we give a brief review of the studies in the area of active plasmonics. In particular, we focus on hybrid J-aggregate/metal nanostructures consisting of J-aggregate excitons and surface plasmon polaritons supported by metallic nanostructures. Two experimental methods: chrip-compensated spectral interferometry and nonlinear pump-probe spectroscopy are introduced. The strong coupling between J-aggregate excitons and SPPs is studied in details by probing both the static optical properties and ultrasfast dynamics of the strongly coupled X-SPP systems. The results reveal that two different energy transfer channels: a coherent resonant dipole-dipole interaction and an incoherent exchange of photons, are coexisting in the hybrid system. Coherent energy exchange, that is, Rabi oscillations between the excitonic and the SPP systems in real time are also investigated. It is found that coherent X-SPP population transfer induces transient oscillations in exciton density, leading to a periodic modulation of the normal mode splitting and thus optical nonlinearity on a 10 fs timescale.

Attosecond dynamics of light-induced resonant hole transfer in high-order-harmonic generation

We present a study of high-order-harmonic generation (HHG) assisted by extreme ultraviolet (XUV) attosecond pulses, which can lead to the excitation of inner-shell electrons and the generation of a second HHG plateau. With the treatment of a one-dimensional model of krypton, based on time-dependent configuration interaction singles (TDCIS) of an effective two-electron system, we show that the XUV-assisted HHG spectrum reveals the duration of the semiclassical electron trajectories. The results are interpreted by the strong-field approximation (SFA) and the importance of the hole transfer during the tunneling process is emphasized. Finally, coherent population transfer between the inner and outer holes with attosecond pulse trains is discussed.

Formation of a molecular ion by photoassociative Raman processes

We show theoretically that it is possible to form a cold molecular ion from a pair of colliding atom and ion at low energy by photoassociative two-photon Raman processes. We explore the possibility of stimulated Raman adiabatic passage from the continuum of ion–atom scattering states to an ionic molecular state. We provide physical conditions under which coherent population transfer is possible in stimulated Raman photoassociation. Our results are important for experimental realization of PA in ion–atom cold collisions.

Tunneling-assisted coherent population transfer and creation of coherent superposition states in triple quantum dots

A scheme is proposed for coherent population transfer and creation of coherent superposition states assisted by one time-dependent tunneling pulse and one time-independent tunneling pulse in triple quantum dots. Time-dependent tunneling, which is similar to the Stokes laser pulse used in traditional stimulated Raman adiabatic passage, can lead to complete population transfer from the ground state to the indirect exciton states. Time-independent tunneling can also create double dark states, resulting in the distribution of the population and arbitrary coherent superposition states. Such a scheme can also be extended to multiple quantum dots assisted by one time-dependent tunneling pulse and more time-independent tunneling pulses.

Efficient polarization of high-angular-momentum systems

We propose methods of optical pumping that are applicable to open, high-angular-momentum transitions in atoms and molecules, for which conventional optical pumping would lead to significant population loss. Instead of applying circularly polarized cw light, as in conventional optical pumping, we propose to use techniques for coherent population transfer (e.g., adiabatic fast passage) to arrange the atoms so as to increase the entropy removed from the system with each spontaneous decay from the upper state. This minimizes the number of spontaneous-emission events required to produce a stretched state, thus reducing the population loss due to decay to other states. To produce a stretched state in a manifold with angular momentum J, conventional optical pumping requires about 2J spontaneous decays per atom, one of our proposed methods reduces this to about log_2(2J), while another of the methods reduces it to about one spontaneous decay, independent of J.

Population transfer driven by far-off-resonant fields.

For a two-level system, it is believed that a far-off-resonant driving cannot help coherent population transfer between two states. In this work, we propose a scheme to implement the coherent transfer with far-off-resonant driving. The scheme works well with both constant driving and Gaussian driving. The total time to finish population transfer is also minimized by optimizing the detuning and coupling constants. We find that the scheme is sensitive to spontaneous emission much more than dephasing. It might find potential applications in X-ray quantum optics and population transfer in Rydberg atoms as well.

Holonomic Quantum Control with Continuous Variable Systems.

Universal computation of a quantum system consisting of superpositions of well-separated coherent states of multiple harmonic oscillators can be achieved by three families of adiabatic holonomic gates. The first gate consists of moving a coherent state around a closed path in phase space, resulting in a relative Berry phase between that state and the other states. The second gate consists of "colliding" two coherent states of the same oscillator, resulting in coherent population transfer between them. The third gate is an effective controlled-phase gate on coherent states of two different oscillators. Such gates should be realizable via reservoir engineering of systems that support tunable nonlinearities, such as trapped ions and circuit QED.