Ultrafast control of coherent population transfer with a train of femtosecond pulse pairs

We investigate the ultrafast control of coherent population transfer in a Λ-type three-level system with a train of pump-Stokes femtosecond pulse pairs, where the pulse sequences can be produced either by optical delay line or by pulse shaping with sinusoidal phase modulation. It is shown that when the pump and Stokes pulses in each pair are applied in the counterintuitive order, similar to that in the stimulated Raman adiabatic passage technique, due to temporal quantum interference (besides optical interference in the case of overlapped subpulses), ultrafast control of coherent population transfer can be achieved by scanning the inter-pair time delay or by changing the sinusoidal phase modulation parameters. This method has potential applications in ultrafast control of chemical reactions and quantum information processing.     

General theory of population transfer by adiabatic rapid passage with intense, chirped laser pulses

We present a general theory of adiabatic rapid passage (ARP) with intense, linearly chirped laser pulses. For pulses with a Gaussian profile and a fixed bandwidth, we derive a rigorous formula for the maximum temporal chirp rate that can be sustained by the pulse. A modified Landau-Zener formula displays clearly the relationships among the pulse parameters. This formula is used to derive the optimal conditions for efficient, robust population transfer. As illustrations of the theory, we present results for two- and four-level systems, and selective vibronic excitation in the I₂ molecule. We demonstrate that population transfer with chirped pulses is more robust and more selective than population transfer with transform-limited pulses. Received 6 September 2000 and Received in final form 25 September 2000     

Efficient coherent population transfer among three states in NO molecules by Stark-Chirped rapid adiabatic passage

We present the experimental demonstration of a novel, efficient, and selective technique to prepare population inversion. The technique is an extension of Stark-chirped rapid adiabatic passage (SCRAP), i.e., SCRAP among three states. In this process a Lambda-type quantum system is driven by two laser pulses, the pump and Stokes pulses, which are appropriately detuned from transition frequencies. A third laser pulse induces a dynamic Stark shift in the upper energy level, and the timing of all three pulses is controlled in order to prepare population inversion between the two lower states in the Lambda-type level scheme. Our data on population transfer in nitric oxide (NO) molecules clearly show that SCRAP among three states provides an advantageous alternative to such techniques as stimulated Raman adiabatic passage.     

Efficient population transfer by delayed pulses despite coupling ambiguity

In traditional schemes of multilevel multilaser excitation, each laser pulse interacts with only one pair of states, and the rotating wave approximation (RWA) is applicable. Here we study the population transfer process in a three-state system when each of the two lasers interacts with each of the pair of states and when the Rabi frequencies characterizing the interaction strengths of the system are comparable to or larger than the difference of the transition frequencies. We show that complete and robust population transfer is possible under conditions more general than those hitherto considered necessary for stimulated Raman adiabatic passage (STIRAP) or for successive π pulses. Using adiabatic Floquet theory we show that successful population transfer can be interpreted as adiabatic passage by means of a transfer state which connects the initial and final states. The Floquet picture offers a convenient interpretation of the population transfer as accompanied by multiple absorption of photons from or emission into the laser fields.     

Stimulated Raman adiabatic passage with temporal pulselets

Stimulated Raman adiabatic passage (STIRAP) is a well established technique whereby two pulses, S preceding P, induce complete population transfer between states 1 and 3 of a three-state chain, 1-2-3. Traditionally, the S and P pulse envelopes are taken as positive (often with Gaussian form of time dependence). However, when the envelope undergoes a sign change during the pulse, as occurs with pulses in which an abrupt phase change of π occurs and whose temporal area (time-integrated Rabi frequency) is zero, then the simple population transfer need not occur. Instead there may occur multiple adiabatic passages, in which the population may ultimately be left in either state 1 (a double STIRAP) or state 3 (a triple STIRAP) or, with suitable pulse delay, in a superposition of these two states. These adiabatic changes offer possibilities to produce final-state probability amplitudes with either positive or negative signs. We here show simulated examples of such behavior, and discuss the adiabatic conditions needed for such excitation to occur.     

Enhancement of coherent population transfer in a double Λ-type four-level system via a train of pulse pairs

We propose a flexible way to significantly enhance population transfer efficiency with a train of time-separated pump-Stokes pulse pairs when the non-adiabatic coupling between two degenerate adiabatic states exists in a double Λ-type four-level system, where the pump and Stokes pulses in each pair can be applied in either counterintuitive or intuitive order. It is shown that the needed Rabi frequency for achieving complete population transfer can be reduced dramatically with the increase of number of pump-Stokes pulse pairs, which results from temporal constructive quantum interference between the sequential transitions and subsequent coherent accumulation; moreover, an arbitrary coherent superposition between the two lower states can be realized by suitably tuning the Rabi frequency and the time delay between each pump-Stokes pair. The method may find applications in control of chemical reactions, quantum optics, and quantum information processing.     

Piecewise adiabatic population transfer in a molecule via a wave packet

We propose a class of schemes for robust population transfer between quantum states that utilize trains of coherent pulses, thus forming a generalized adiabatic passage via a wave packet. We study piecewise stimulated Raman adiabatic passage with pulse-to-pulse amplitude variation, and piecewise chirped Raman passage with pulse-to-pulse phase variation, implemented with an optical frequency comb. In the context of production of ultracold ground-state molecules, we show that with almost no knowledge of the excited potential, robust high-efficiency transfer is possible.     

Quantum information transfer with Cooper-pair box qubits in circuit QED

We propose a feasible scheme to transfer quantum information with Cooper-pair box qubits arrayed in a circuit QED. Qubits interact with a quantum data bus generated by a one-dimensional transmission line resonator. Based on the Raman adiabatic passage, the cavity bus-assisted quantum population transfer between any selected pair of qubits can be controlled by addressing the applied gate pulses. Therefore, the scheme provides the possibility for effectively implementing scalable quantum information transfer with Josephson devices.     

Rapid adiabatic passage without level crossing

We present a method for achieving complete population transfer in a two-state quantum system via adiabatic time evolution in which, contrary to conventional rapid adiabatic passage produced by chirped pulses, there occurs no crossing of diabatic energy curves: there is no sign change of the detuning. Instead, we use structured pulses, in which, in addition to satisfying conditions for adiabatic evolution, there occurs a sign change of the Rabi frequency when the detuning is zero. We present simulations that offer simple geometrical interpretation of the two-dimensional motion of the Bloch vector for this system, illustrating how both complete population inversion and complete population return occur for different choices of structured pulses.     

Efficient Population Transfer in a Λ-Type Quantum System Coupled to a Gold Nanoparticle Using STIRAP Shortcuts

A theoretical investigation on the population transfer in a Λ-type quantum system near a spherical gold nanoparticle under application of two stimulated Raman adiabatic passage (STIRAP) shortcuts and efficiency comparison with conventional STIRAP. It combines the density matrix approach for system dynamics, with classical electromagnetic calculations used to obtain the modified electric field amplitudes of the applied pulses and the Purcell factor of the quantum system due to the presence of the nanoparticle. The efficiency of population transfer is investigated by varying the distance between the quantum system and the nanoparticle, the free-space decay rate of quantum states, the mutual polarization, and the Rabi frequencies of each STIRAP shortcut pulses. In all cases, at least one of the applied shortcuts is more efficient than conventional STIRAP, while in most cases both perform better. When the pump and Stokes fields of the shortcuts have radial and tangential polarizations with respect to the nanoparticle surface, respectively, high transfer efficiency is obtained for small distances of the quantum system to the nanoparticle, moderate free space decay rates and large Rabi frequencies of the fields, while when the pulse polarizations are interchanged, the transfer becomes highly efficient only at large distances.     

Acoustic topological adiabatic passage via a level crossing

Stimulated adiabatic passage has been extensively studied to achieve robust and selective population transfer in quantum systems. Recently, the quantum-classic analogy has been rapidly developing and can be considered responsible for the implementation of the adiabatic transfer of sound energy in cavity chain systems. In this article, we investigate the adiabatic transfer of sound energy between two topological end states in the Su-Schrieffer-Heeger(SSH) cavity chain, which can be considered to be the acoustic analog of the quantum chirped-pulse excitation. The topological adiabatic passage in SSH cavity chain has two categories. When the single-cavity resonance frequencies on the sublattices A and B in the SSH cavity chain do not switch their spectrum positions, the topologically protected adiabatic evolution results in the returning passage of the sound excited in one end cavity. When a level crossing with single-cavity resonance frequencies on the sublattices A and B exhibits switch in the frequency spectrum, acoustic energy is observed to be topologically pumped between the two end cavities of the SSH chain.     

Robust quantum dot exciton generation via adiabatic passage with frequency-swept optical pulses

The energy states in semiconductor quantum dots are discrete as in atoms, and quantum states can be coherently controlled with resonant laser pulses. Long coherence times allow the observation of Rabi flopping of a single dipole transition in a solid state device, for which occupancy of the upper state depends sensitively on the dipole moment and the excitation laser power. We report on the robust population inversion in a single quantum dot using an optical technique that exploits rapid adiabatic passage from the ground to an excited state through excitation with laser pulses whose frequency is swept through the resonance. This observation in photoluminescence experiments is made possible by introducing a novel optical detection scheme for the resonant electron hole pair (exciton) generation.     

Digitally stimulated Raman passage by deep reinforcement learning

Preparing an arbitrary preselected coherent superposition of quantum states finds widespread application in physics, including initialization of trapped ion and superconductor qubits in quantum computers. Both fractional and integer stimulated Raman adiabatic passage involve smooth Gaussian pulses, designed to grant adiabaticity, so to keep the system in an eigenstate constituted only of the initial and final states. We explore an alternative method for discovering appropriate pulse sequences based on deep reinforcement learning algorithms and by imposing that the control laser can be only either on or off instead of being continuously amplitude-modulated. Despite the adiabatic condition is violated, we obtain fast and flexible solutions for both integer and fractional population transfer. Such method, consisting of a Digital Stimulated Raman Passage (D-STIRaP), proves to be particularly effective when the system is affected by dephasing therefore providing an alternative path towards control of noisy quantum states, like trapped ions and superconductor qubits.     

Floquet theory for short laser pulses

We develop adiabatic perturbation theory for quantum systems responding to short laser pulses, with or without a frequency chirp. Our approach rests on lifting the time-dependent Schr?dinger equation to an extended Hilbert space, then applying standard perturbational techniques to Floquet states in this extended space, and finally projecting back to the physical Hilbert space. The same strategy also allows us to construct superadiabatic bases for monitoring the quantum evolution in the course of a pulse. These bases provide a diagnostic tool for improving the efficiency of pulse-induced population transfer. The formalism is applied to the selective excitation of molecular vibrational states by chirped laser pulses, which exploit either successive single-photon resonances or a multiphoton resonance, and by a STIRAP-like process. Received: 23 June 1998 / Revised: 18 August 1998 / Accepted: 25 August 1998     

Dependence of adiabatic population transfer on pulse profile

Control of population transfer by rapid adiabatic passage has been an established technique wherein the exact amplitude profile of the shaped pulse is considered to be insignificant. We study the effect of ultrafast shaped pulses for two-level systems, by density-matrix approach. However, we find that adiabaticity depends simultaneously on pulse profile as well as the frequency modulation under non-resonant conditions     

Stimulated Raman adiabatic passage via the ionization continuum in helium: Experiment and theory

We experimentally demonstrate coherent population transfer, driven by stimulated Raman adiabatic passage (STIRAP) between two bound quantum states, coupled via a continuum of states. We present extended numerical and experimental investigations on population transfer from the metastable state 2s ¹S₀ to the excited state 4s ¹S₀ in metastable helium atoms. While techniques based on incoherent excitation do not permit any population transfer via rapidly decaying continuum states, our data indicate a maximum transfer efficiency of 20% in coherent excitation by STIRAP. We study the transfer efficiency with respect to the relevant experimental parameters.     

Phase evolution of the reemitted field in the semiconductor quantum wells under the femtosecond pulse train intersubband excitation

Property of the phase of the reemitted field in the semiconductor quantum wells (QWs) excited by femtosecond pulse train is investigated. It is shown that the phase evolution of the reemitted field is controlled by the relative phase between the successive pulses of the incident train. For all the odd pulses excitation,the reemitted field is from out-of-phase to in-phase, then again to out-of-phase with the incident pulses,whereas for all the even pulses excitation, the situation is the opposite, i.e., it is from in-phase to out-of-phase, then again to in-phase with the incident pulses.     

Inversion in an extended three-level medium produced by adiabatic population transfer

Features of the adiabatic population transfer are studied with the spatial evolution of interacting pulses propagating in an optically dense medium of three-level Λ-atoms taken into account. A self-consistent analytical solution describing the spatial-temporal dynamics of interacting short pulses under the conditions of adiabatic population transfer is constructed in the adiabatic approximation with consideration for the first nonadiabatic correction. Practically complete inversion on a forbidden transition determined by coherent (adiabatic) population transfer is shown to take place over a length of the medium, which may exceed the absorption length of a weak probing pulse in the absence of control radiation on the adjacent transition by several orders of magnitude.     

Stimulated Raman adiabatic passage in fields with stochastic amplitudes

A theoretical analysis is presented of the effect of correlation between fluctuations of laser pulse amplitudes on population transfer between the states of a three-level atom coupled by the laser field. The carrier frequencies of the pulses are tuned to resonance with the transitions between the ground and excited states, |〈 and | 2〈, and the excited and metastable states, |2〈 and |3〈, in a lambda-type configuration. The laser pulses are timed so that population transfer between states |1〈 and | 3〈 is made possible by stimulated Raman adiabatic passage (STIRAP) in the absence of fluctuations. STIRAP does not occur when the laser fields are not correlated. When the fluctuations of one pulse amplitude duplicate those of the other, STIRAP can be observed for pulse amplitudes larger than those required in the absence of fluctuations.     

Multiband Adiabatic Inversion Pulses

The conditions necessary to obtain multiple adiabatic population inversion at different frequencies in a two-level system are defined. It is shown how any pulse that produces adiabatic inversion in a single frequency band can be modified to become a multiband adiabatic inversion pulse. Using Floquet formalism, the interaction between the different inversion bands is described and shown to create effective nonlinear irradiation fields. By controlling the reference phase of the single-inversion-frequency-band pulses, these effective irradiation fields can be minimized or canceled. These pulses can be used for multiple selective excitation or selective population inversion in coherent spectroscopy. NMR experiments confirming the theoretical predications are shown. The experimental results agree very well with the theoretical predictions.