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Journal of Modern Optics

Frequency domain control of quantum state singlet/triplet character and prospects for an all-optical spin switch

Ergin H. Ahmed, A. M. Lyyra

Published Sep 5, 2013• 3 citations
Publisher

Abstract

In recent years, quantum optics has been expanded from atomic to molecular systems despite much weaker oscillator strengths and complex relaxation pathways that have presented serious challenges in the past. The richness of molecular excitation pathways and the variety of molecular interactions has made it possible to develop novel applications in this field. We have demonstrated how the Autler–Townes effect can be used to control molecular angular momentum alignment and how the Autler–Townes split line shape, combined with accurate control-laser electric field amplitude measurement, can be used to map the absolute magnitude of the molecular internuclear distance dependent electronic transition dipole moment function. In addition, the electric field amplitude in the control laser Rabi frequency can be used as a ‘tuning’ mechanism for the mixing coefficients of energy levels that are weakly perturbed by the spin–orbit interaction, i.e. to control the valence electron spin polarization and the spin multipli...

DOI
10.1080/09500340.2013.827248

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Abstract Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.

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In recent years, quantum optics has been expanded from atomic to molecular systems despite much weaker oscillator strengths and complex relaxation pathways that have presented serious challenges in the past. The richness of molecular excitation pathways and the variety of molecular interactions has made it possible to develop novel applications in this field. We have demonstrated how the Autler–Townes effect can be used to control molecular angular momentum alignment and how the Autler–Townes split line shape, combined with accurate control-laser electric field amplitude measurement, can be used to map the absolute magnitude of the molecular internuclear distance dependent electronic transition dipole moment function. In addition, the electric field amplitude in the control laser Rabi frequency can be used as a ‘tuning’ mechanism for the mixing coefficients of energy levels that are weakly perturbed by the spin–orbit interaction, i.e. to control the valence electron spin polarization and the spin multipli...
We have demonstrated quantum control of the spin-orbit interaction based on the Autler-Townes (ac-Stark) effect in a molecular system using a cw optical field. We show that the enhancement of the spin-orbit interaction between a pair of weakly interacting singlet-triplet rovibrational levels, G (1)Π(g)(v=12,J=21,f)-1 (3)Σ(g)(-)(v=1,N=21,f), separated by 750 MHz in the lithium dimer, depends on the Rabi frequency (laser power) of the control laser. The increase in the spin-orbit interaction due to the control field is observed as a change in the spin character of the individual components of the perturbed pair.
We have demonstrated Autler-Townes splitting in molecular lithium using continuous wave triple resonance spectroscopy. The Autler-Townes split double resonance lineshape consists of a superposition of several narrower twin peaks, one for each | M j |. The splitting is proportional to | M j | enabling separation of the individual Mj peaks. Thus, excitation of an individual magnetic sublevel can be used to align the angular momentum of nonpolar molecules all-optically. We also propose a novel quantum control scheme based on using a coupling laser to create dressed states of controllable molecular character. Preliminary calculations are presented for variable singlet triplet character.
This paper describes an extension of the familiar coherence effects from atomic systems to the molecular regime. Such effects are inherent in the interaction of multiple laser fields with molecular systems. We have observed Autler–Townes splitting and the AC Stark shift in diatomic Lithium using the continuous wave all-optical triple resonance (AOTR) techniques. By using the Autler–Townes effect, we have partially resolved the magnetic sublevels of a molecular rovibrational level in a Doppler broadened sample, allowing all-optical alignment of the angular momentum in excited states of nonpolar molecules. The Autler–Townes effect in a molecular system extends the rovibrational state selectivity of the AOTR excitation technique to magnetic sublevels. PACS Nos.: 33.40tf, 42.50Hz
Control of molecular angular momentum orientation enables state-resolved studies of molecular interactions and provides a basis for quantum information processing. Here we propose all-optical Autler-Townes state-selective adiabatic passage (ASAP) to prepare molecules in a single ∣J,M⟩|J,M\rangle∣J,M⟩ sublevel. An Autler-Townes branch created by a strong coupling field is selectively populated and adiabatically mapped onto the target vibrational state. We resolve detuning-dependent rovibrational Autler-Townes splitting in 13^{13}13CO2_22​, establishing the spectroscopic basis for the selective excitation of the target dressed branch. The density-matrix model calibrated by these spectra predicts transfer approaching 90\%. The scheme can exploit millisecond vibrational radiative lifetimes within the electronic ground state and extend to polar and nonpolar molecules with infrared-active vibrational modes.
Abstract Rabi oscillations are periodic modulations of populations in two-level systems interacting with a time-varying field1. They are ubiquitous in physics with applications in different areas such as photonics2, nano-electronics3, electron microscopy4 and quantum information5. While the theory developed by Rabi was intended for fermions in gyrating magnetic fields, Autler and Townes realized that it could also be used to describe coherent light–matter interactions within the rotating-wave approximation6. Although intense nanometre-wavelength light sources have been available for more than a decade7–9, Rabi dynamics at such short wavelengths has not been directly observed. Here we show that femtosecond extreme-ultraviolet pulses from a seeded free-electron laser10 can drive Rabi dynamics between the ground state and an excited state in helium atoms. The measured photoelectron signal reveals an Autler–Townes doublet and an avoided crossing, phenomena that are both fundamental to coherent atom–field interactions11. Using an analytical model derived from perturbation theory on top of the Rabi model, we find that the ultrafast build-up of the doublet structure carries the signature of a quantum interference effect between resonant and non-resonant photoionization pathways. Given the recent availability of intense attosecond12 and few-femtosecond13 extreme-ultraviolet pulses, our results unfold opportunities to carry out ultrafast manipulation of coherent processes at short wavelengths using free-electron lasers.