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New Journal of Physics

Stimulated Raman adiabatic passage with two-color x-ray pulses

Antonio Picón, J. Mompart, Stephen H. Southworth

Published Aug 19, 2015• 18 citations
Publisher

Abstract

Recent techniques in x-ray free electron lasers allow the generation of highly coherent, intense x-ray pulses with time lengths on the order of femtoseconds. Here we explore the possibilities of using such x-ray pulses to control matter based on coherence. In particular we propose a theoretical scheme to perform stimulated Raman adiabatic passage in the x-ray regime by using inner-hole excited states. Numerical results in two well-known systems, the neon atom and the carbon monoxide molecule, show a robust control of population transfer. In the molecule, vibrational selectivity is achieved with femtosecond x-ray pulses. This work supports the possibility of using two-color x-ray pulses for coherent control.

DOI
10.1088/1367-2630/17/8/083038

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Recent techniques in x-ray free electron lasers allow the generation of highly coherent, intense x-ray pulses with time lengths on the order of femtoseconds. Here we explore the possibilities of using such x-ray pulses to control matter based on coherence. In particular we propose a theoretical scheme to perform stimulated Raman adiabatic passage in the x-ray regime by using inner-hole excited states. Numerical results in two well-known systems, the neon atom and the carbon monoxide molecule, show a robust control of population transfer. In the molecule, vibrational selectivity is achieved with femtosecond x-ray pulses. This work supports the possibility of using two-color x-ray pulses for coherent control.
Abstract Coherent control uses interference between quantum pathways to enhance or suppress transitions to a target quantum state. In stimulated Raman excitation, such control can be achieved through interference between two indistinguishable pathways connecting the same initial and final states, with the relative phase between the pathways modulating the population transfer to the final state. Extending this strategy to the extreme ultraviolet (XUV) and X-ray regimes would enable control of ultrafast electronic dynamics and site-selective core excitations. However, Raman coupling at short wavelengths competes with photoionization and intermediate-state decay, whereas intense fields with stable and adjustable relative phases remain difficult to produce. Here we use two-colour pulses from a seeded coherent free-electron laser to excite helium from its ground state to a bound metastable state via stimulated XUV Raman excitation. We implement phase-coherent control by creating two interfering Raman pathways through the ionization continuum and modulate the transferred population by varying their relative phases. Blocking one pathway removes the modulation, confirming its interferometric origin, and time-dependent Schrödinger equation calculations reproduce the measured phase dependence. Our results establish phase-controlled stimulated Raman excitation in the XUV regime, providing a strategy for the coherent control of atomic and molecular processes at short wavelengths.
The controlled transfer of nuclear state population using two x-ray laser pulses is investigated theoretically. The laser pulses drive two nuclear transitions in a nuclear three-level system facilitating coherent population transfer via the quantum optics technique of stimulated Raman adiabatic passage. To overcome present limitations of the x-ray laser frequency, we envisage accelerated nuclei interacting with two copropagating or crossed x-ray laser pulses in a three-beam setup. We present a systematic study of this setup providing both pulse temporal sequence and laser pulse intensity for optimized control of the nuclear state population. The tolerance for geometrical parameters such as laser beam divergence of the three-beam setup as well as for the velocity spread of the nuclear beam are studied and a two-photon resonance condition to account for experimental uncertainties is deduced. This additional condition gives a less strict requirement for the experimental implementation of the three-beam setup. Present experimental state of the art and future prospects are discussed.
Nuclear coherent population transfer to the 229m^{229m}229mTh isomer using x-ray pulses
Population of the 8 eV 229m^{229m}229mTh isomer via the second nuclear excited state at 29.19 keV by means of coherent x-ray pulses is investigated theoretically. We focus on two nuclear coherent population transfer schemes using partially overlapping x-ray pulses known from quantum optics: stimulated Raman adiabatic passage (STIRAP), and successive πππ pulses. Numerical results are presented for three possible experimental setups. Our results identify the Gamma Factory as the most promising scenario, where two ultraviolet pulses combined with relativistically accelerated ions deliver the required intensities for efficient isomer population. Our simulations require knowledge of the in-band and cross-band nuclear transition probabilities. We give theoretically predicted values for the latter and discuss them in the context of recent experiments.
A novel chirped pulse control scheme is presented based on Coherent Anti-Stokes Raman Spectroscopy (C-CARS) aiming at maximizing the vibrational coherence in atoms and molecules. The scheme utilizes chirping of the three incoming pulses, the pump, the Stokes and the probe, in the four-wave mixing process of C-CARS to fulfill the adiabatic passage conditions. The derivation of the scheme is based on simplifying the four-level system into a 'super-effective' two level system via rotating wave approximation and adiabatic elimination of the excited state manifold. The robustness, spectral selectivity and adiabatic nature of C-CARS method may prove useful for sensing, imaging, and detection. It is demonstrated that the selectivity in excitation of vibrational degrees of freedom can be controlled by carefully choosing the spectral chirp rate of the pulses. The C-CARS control scheme is applied to a surrogate methanol molecule to generate an optimal anti-Stokes signal backscattered from a cloud of molecules a kilometer away. The theory is based on the solution of the coupled Maxwell-Liouville von Neumann equations and focuses on the quantum effects induced in the target molecules by the control pulse trains. The propagation effects of pulses through the medium are evaluated and the buildup of the molecular-specific anti-Stokes signal is demonstrated numerically. A deep learning technique, using Convolutional Neural Networks (CNN), is implemented to characterize the control pulses and evaluate time-dependent phase characteristics from them. The effects of decoherence induced by spontaneous decay and collisional dephasing are also examined. Additionally, we present the technique of Fractional Stimulated Raman Adiabatic Passage (F-STIRAP) and demonstrate that it can be utilized for remote detection in a multi-level system by creation of a maximally coherent superposition state.
We discuss the properties of a simple and robust scheme for preparing atoms and molecules in an arbitrary preselected coherent superposition of quantum states - fractional stimulated Raman adiabatic passage (fractional STIRAP) - first proposed by Marte et al (1991 Phys. Rev. A 44 R4118). As in STIRAP, the Stokes pulse arrives before the pump pulse, but unlike STIRAP, here the two pulses terminate simultaneously, while maintaining a constant ratio of amplitudes. We extend earlier research and suggest a realization of this scheme with two smoothly varying delayed laser pulses (which can be derived from a single laser), the parameters of the created superposition being controlled by the polarization of the delayed pulse. Furthermore, we provide simple analytic estimates of the robustness of this process against variations in the laser intensity, laser frequency and pulse delay. Finally, we discuss an extension to multistate systems which provides a possibility for creating coherent superpositions of more than two states.
We theoretically study the generation of coherence in generalized two-level atoms with hyperfine structure by utilizing the detuning-induced stimulated Raman adiabatic passage (D-STIRAP). As expected, the degree of attainable coherence between the ground and excited states cannot be as large as that for the ideal two-level atoms without hyperfine structure. However, we find that the substantial degree of coherence can still be produced with small modulations, and the modulation period is essentially determined by the hyperfine splittings in the ground and excited states. The D-STIRAP scheme in generalized two-level atoms is sufficiently robust against the various parameters such as intensities of lasers, initial detuning, time delay between the laser pulses, and Doppler broadening. As a specific example, we show realistic results for the D1{D}_{1}D1​ transition of Na.