Population transfer via adiabatic passage in the rubidium quantum ladder system

Maas, D. J. H. C.; Rella, C.; Antoine, Philippe; Toma, E. S.; Noordam, L. D.

doi:10.1103/physreva.59.1374

Cited by 46 publications

(26 citation statements)

References 12 publications

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“…Finally, an issue that should be addressed is the quantum interference between sequential and direct multiphoton paths that have been reported in other systems (23)(24)(25). This effect results in oscillations in the signal as a function of the pump chirp.…”

Section: ]mentioning

confidence: 99%

Coherent vibrational climbing in carboxyhemoglobin

Ventalon

Fraser

Vos

et al. 2004

Proc. Natl. Acad. Sci. U.S.A.

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We demonstrate vibrational climbing in the CO stretch of carboxyhemoglobin pumped by midinfrared chirped ultrashort pulses. By use of spectrally resolved pump-probe measurements, we directly observed the induced absorption lines caused by excited vibrational populations up to v ‫؍‬ 6. In some cases, we also observed stimulated emission, providing direct evidence of vibrational population inversion. This study provides important spectroscopic parameters on the CO stretch in the strong-field regime, such as transition frequencies and dephasing times up to the v ‫؍‬ 6 to v ‫؍‬ 7 vibrational transition. We measured equally spaced vibrational transitions, in agreement with the energy levels of a Morse potential up to v ‫؍‬ 6. It is interesting that the integral of the differential absorption spectra was observed to deviate far from zero, in contrast to what one would expect from a simple onedimensional Morse model assuming a linear dependence of dipole moment with bond length.T he recent availability of ultrashort and intense midinfrared pulses in a compact setup (1) provides a convenient means for controlling the nuclear motion of molecules (2). With infrared pulses, only vibrational transitions are addressed while the molecule remains in its electronic ground state during the entire interaction. This makes such an approach particularly suited to complex systems such as proteins. Another fascinating possibility opened up by infrared vibrational control is the prospect of exploring the potential energy surface far from the harmonic region up to the transition state of intraprotein reactions.Coherent vibrational climbing consists of exciting a molecular vibration with an ultrashort midinfrared pulse, the broadband spectrum of which encompasses several vibrational transitions of the molecule. Indeed, these transition frequencies become smaller and smaller while climbing the ladder because of the molecular anharmonicity. Therefore, the climbing efficiency can be increased dramatically when using a negatively chirped pulse so that its high-frequency components, resonant with the lower transitions of the ladder, precede its low-frequency components, resonant with the upper transitions of the ladder. Coherent vibrational climbing can be viewed also as a rapid adiabatic passage leading to efficient excitation of the upper vibrational states, with an efficiency that in theory can be close to 100% because of the coherent nature of the interaction. Vibrational climbing has been demonstrated in small molecules, such as W(CO) 6 (3-5), NO (6), CO adsorbed on a Ru (001) surface (7), Cr(CO) 6 (8), Mo(CO) 6 (5), Fe(CO) 5 (5), and CH 2 N 2 (9). In this article, we report on the demonstration of coherent vibrational climbing in a biological system, carboxyhemoglobin (HbCO). This system was chosen rather than carboxymyoglobin, in which different CO-bound configurations result in an inhomogeneous broadening of the absorption line (10). Experimental MethodsThe 800-nm pulses produced by a titanium͞sapphire regenerative amplifier (Hurrican...

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Section: ]mentioning

confidence: 99%

Coherent vibrational climbing in carboxyhemoglobin

Ventalon

Fraser

Vos

et al. 2004

Proc. Natl. Acad. Sci. U.S.A.

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“…In the context of semiconductor quantum dots adiabatic population transfer has been induced by a slow variation of the electrostatically defined confinement potential [14]. For applications in atomic physics and chemistry for quantum states separated by frequencies in the optical domain, chirped laser pulses, in strong analogy to NMR, have been used to induce complete population transfer via adiabatic passage [12,15,16]. Our experiments demonstrate the power of adiabatic population transfer between individual quantum states in condensed matter, paving the way for stimulated Raman adiabatic passage (STIRAP) [12,17], efficient spin state preparation [18,19] and quantum condensation of excitons in a microcavity [20].…”

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confidence: 99%

Robust Quantum Dot Exciton Generation via Adiabatic Passage with Frequency-Swept Optical Pulses

et al. 2011

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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 preparation of a quantum state 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. Photon correlation measurements along with resonant laser scattering have established the atom-like character of the interband transitions in quantum dots [1][2][3]. Excitation of a two level system by a short, intense laser pulse can induce an oscillation of the system between the upper and lower state during the pulse, at the Rabi frequency Ω(t) = µA(t)/ where µ is the dipole moment of the transition and A(t) the electric field envelope of the laser pulse. Any quantum state (qubit) manipulation scheme benefits from the long coherence times in quantum dots [4] and necessitates fast and robust initial state preparation [5][6][7]. In principle a two level system can be initialised in the upper state with a maximum fidelity of 100% if the laser power is optimised in order to induce exactly half a Rabi oscillation during the pulse duration, a so-called π pulse [8][9][10]. Although Rabi oscillations observed in a single dot or for individual atoms [11] are a beautiful example of strong coupling between laser light and a single dipole, this commonly used technique presents two major drawbacks: (i) the upper state population is highly sensitive to fluctuations in the system, such as laser power, and (ii) in measurements on dot ensembles, an inhomogeneous distribution of dipole moments and transition energies among dots requires different laser intensities and frequencies for inducing a population transfer of the dot ensemble.Here we show that these drawbacks can be overcome by inducing an adiabatic passage with frequency-swept laser pulses. Unlike Rabi cycling, adiabatic passage is robust against small-to-moderate variations in the laser * Corresponding author : urbaszek@insa-toulouse.fr intensity, detuning, dipole moment and interaction time [12]. Chirped radiofrequency (RF) pulses are commonly used in nuclear magnetic resonance (NMR) based imaging [13]. In the context of semiconductor quantum dots adiabatic population transfer has been induced by a slow variation of the electrostatically defined confinement potential [14]. For applications in atomic physics and chemistry for quantum states separated by frequencies in the optical domain, chirped laser pulses, in strong analogy to NMR, have been used to induce complete population transfer via...

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“…As the intensity is increased, the counterintuitive two-photon absorption becomes efficient for negative chirp. With chirped ultrashort pulses, the population transfer process is a variant of the wellknown rapid adiabatic passage (RAP) technique [17,19,20]. The excited-state fluorescence was significantly reduced near the zero-GDD axis, where such pulse shapes produce peak intensities high enough to ionize the atom.…”

Section: Resultsmentioning

confidence: 99%

Strong-field spatiotemporal ultrafast coherent control in three-level atoms

et al. 2010

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Simple analytical approaches for implementing strong field coherent control schemes are often elusive due to the complexity of the interaction between the intense excitation field and the system of interest. Here, we demonstrate control over multiphoton excitation in a three-level resonant system using simple, analytically derived ultrafast pulse shapes. We utilize a two-dimensional spatiotemporal control technique, in which temporal focusing produces a spatially dependent quadratic spectral phase, while a second, arbitrary phase parameter is scanned using a pulse shaper. In the current work, we demonstrate weak-to-strong field excitation of 85 Rb, with a π phase step and the quadratic phase as the chosen control parameters. The intricate dependence of the multilevel dynamics on these parameters is exhibited by mapping the data onto a two-dimensional control landscape. Further insight is gained by simulating the complete landscape using a dressed-state, time-domain model, in which the influence of individual shaping parameters can be extracted using both exact and asymptotic time-domain representations of the dressed-state energies.

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Population transfer via adiabatic passage in the rubidium quantum ladder system

Cited by 46 publications

References 12 publications

Coherent vibrational climbing in carboxyhemoglobin

Coherent vibrational climbing in carboxyhemoglobin

Robust Quantum Dot Exciton Generation via Adiabatic Passage with Frequency-Swept Optical Pulses

Strong-field spatiotemporal ultrafast coherent control in three-level atoms

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