Temporal Coherent Control in Two-Photon Transitions: From Optical Interferences to Quantum Interferences

Blanchet, Valérie; Nicole, C.; Bouchène, M. A.; Girard, B.

doi:10.1103/physrevlett.78.2716

Cited by 190 publications

(126 citation statements)

References 18 publications

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“…Very rapid, suboptical-cycle modulations in the photoelectron and D + 2 yields result from the combination of optical interferences (two IR pulses) and quantum interferences of electronic wavepackets (i.e., 9ω + ω and 11ω − ω interfering pathways), as the phase of the control IR pulse changes relative to the pump VUV + IR pulse. Half-a-cycle periodicity suggests that the two-pathway quantum interferences play an important role in this particular case (29). The deep, full-cycle modulation of the dissociative D + yield is simply a result of the optical interferences between the pump and control IR pulses (both 30 fs long) that lead to bond-softening of the ground state of D + 2 and ionization of the D p 2 excited states ∼10 fs after the pump pulse.…”

Section: Methodsmentioning

confidence: 99%

Attosecond vacuum UV coherent control of molecular dynamics

Ranitovic

Hogle

Rivière

et al. 2014

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

122

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High harmonic light sources make it possible to access attosecond timescales, thus opening up the prospect of manipulating electronic wave packets for steering molecular dynamics. However, two decades after the birth of attosecond physics, the concept of attosecond chemistry has not yet been realized; this is because excitation and manipulation of molecular orbitals requires precisely controlled attosecond waveforms in the deep UV, which have not yet been synthesized. Here, we present a unique approach using attosecond vacuum UV pulse-trains to coherently excite and control the outcome of a simple chemical reaction in a deuterium molecule in a non-Born-Oppenheimer regime. By controlling the interfering pathways of electron wave packets in the excited neutral and singly ionized molecule, we unambiguously show that we can switch the excited electronic state on attosecond timescales, coherently guide the nuclear wave packets to dictate the way a neutral molecule vibrates, and steer and manipulate the ionization and dissociation channels. Furthermore, through advanced theory, we succeed in rigorously modeling multiscale electron and nuclear quantum control in a molecule. The observed richness and complexity of the dynamics, even in this very simplest of molecules, is both remarkable and daunting, and presents intriguing new possibilities for bridging the gap between attosecond physics and attochemistry.chemical dynamics | electron dynamics | ultrafast T he coherent manipulation of quantum systems on their natural timescales, as a means to control the evolution of a system, is an important goal for a broad range of science and technology, including chemical dynamics and quantum information science. In molecules, these timescales span from attosecond timescales characteristic of electronic dynamics, to femtosecond timescales characteristic of vibrations and dissociation, to picosecond timescales characteristic of rotations in molecules. With the advent of femtosecond lasers, observing the transition state in a chemical reaction (1), and controlling the reaction itself, became feasible. Precisely timed femtosecond pulse sequences can be used to selectively excite vibrations in a molecule, allow it to evolve, and finally excite or deexcite it into an electronic state not directly accessible from the ground state (2). Alternatively, interferences between different quantum pathways that end up in the same final state can be used to control the outcome of a chemical reaction (3)(4)(5)(6)(7)(8)(9).In recent years, coherent high harmonic sources with bandwidths sufficient to generate either attosecond pulse trains or a single isolated attosecond pulses have been developed that are also perfectly synchronized to the driving femtosecond laser (10-12). This new capability provides intriguing possibilities for coherently and simultaneously controlling both the electronic and nuclear dynamics in a molecule in regimes where the BornOppenheimer approximation is no longer valid, to select specific reaction pathways or products. Here...

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Section: Methodsmentioning

confidence: 99%

Attosecond vacuum UV coherent control of molecular dynamics

Ranitovic

Hogle

Rivière

et al. 2014

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

122

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“…To single out some special results in the extremely broad field of interference, we point to recent observations using two-photon pulse transition [94] in which a differentiation was achieved between interferences due to temporal overlap (with finite pulse-width) and quantum interference caused by delay. The (component-specific) topological phase in wave functions has been measured, following the proposal of Berry in [9], by neutron interferometry in a number of works, e.g., [123,124] with continual improvements in the technique.…”

Section: Aspects Of Phase In Moleculesmentioning

confidence: 99%

“…In some recently studied cases these might be a superposition of a good ten or so energy eigen-states. Thanks to the availability of short, femtosecond laser pulses both the control of reactions by coherent light ( [16], [84]- [94]) and the probing of phases in a wave packet are now experimental possibilities ( [19], [95] - [97]). With short duration excitations the initial form of the wave packet is a real "doorway state" ( [98]- [100]) and this develops phases for each of its component amplitudes as the wave-packet evolves.…”

Section: Introduction and Preview Of The Chaptermentioning

confidence: 99%

Complex States of Simple Molecular Systems

Englman¹,

Yahalom²

2002

Advances in Chemical Physics

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A review is given of phase properties in molecular wave functions, composed of a number of (and, at least, two) electronic states that become degenerate at some nearby values of the nuclear configuration. Apart from discussing phases and interference in classical (non-quantal) systems, including light-waves, the review looks at the constructability of complex wave functions from observable quantities ("the phase problem"), at the controversy regarding quantum mechanical phase-operators, at the modes of observability of phase and at the role of phases in some non-demolition measurements. Advances in experimental and (especially) theoretical aspects of Aharonov-Bohm and topological (Berry) phases are described, including those involving two-electron and relativistic systems. Several works in the phase control and revivals of molecular wave-packets are cited as developments and applications of complex-function theory. Further topics that this review touches on are: coherent states, semiclassical approximations and the Maslov index. The interrelation between time and the complex state is noted in the contexts of time delays in scattering, of time-reversal invariance and of the existence of a molecular time-arrow.When the stationary Born-Oppenheimer description for nearly degenerate state is regarded as "embedded" in a broader dynamic formulation, namely through solution of the time dependent Schrödinger equation, the wave function becomes necessarily complex. The analytic behavior of this function in the complex time-plane can be exploited to gain information about the connection between phases and moduli of the componentamplitudes. One form of this connection are a pair of reciprocal (Kramers-Kronig type) relations in the complex time-domain. These show that certain phase changes in a component amplitude (such as, e.g., lead to a non-zero Berry-phase) require changes in the amplitude-moduli, too, and imply degeneracies of the electronic state.The subject of conical degeneracy, or intersection, of adjacent potential surface is extended to nonlinear nuclear-electronic coupling, which can then result in multiple conical degeneracies on a nuclear coordinate plane. We treat cases of double and fourfold intersections, the latter under trigonal symmetry, and employ an analytic-graphical phase tracing method to obtain the resulting Berry phases as the system circles around some or all of the degeneracy points. These phases can take up values that are all integral multiples of π, with integers that vary with the physical situation (or with the model postulated for it).A further type of invariance, with respect to gauge transformation, is also tied to the complex form of the wave function. For a many-component state this leads to a consideration of tensorial (Yang-Mills type) fields F for molecular systems. It is shown that it is the truncation of the Born-Oppenheimer electron-nuclear superposition that generates the molecular Yang-Mills fields.The equations of motion for the nuclear degrees of freedom are derived from a Lagr...

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“…The potential of phase locked pulse sequences as a novel spectroscopic tool was demonstrated on single-photon molecular transitions [34] and discussed in [35]. Later, shaped weak field pulses were employed in order to control multi-photon transitions in atoms [36][37][38][39], molecules [40] and solid state systems [41,42]. It was pointed out that subtle differences due to the relative optical phase either produced by optical phase shifts or time delay [43,44] can control the outcome of the experiment.…”

Section: Pulse Sequence Experimentsmentioning

confidence: 99%

Strong field quantum control by selective population of dressed states

Wollenhaupt

Präkelt

Sarpe-Tudoran

et al. 2005

J. Opt. B: Quantum Semiclass. Opt.

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We study the dynamics of potassium atoms in intense laser fields using femtosecond phase-locked pulse pairs in order to extract physical mechanisms of strong field quantum control. The structure of the Autler-Townes (AT) doublet in the photoelectron spectra is measured to analyse transient processes. The analysis shows that the physical mechanism is based on the selective population of dressed states (SPODS). Experimental results of closed loop optimization of SPODS are presented in addition. Applications to decoherence measurements with implications for quantum information are also proposed.

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Temporal Coherent Control in Two-Photon Transitions: From Optical Interferences to Quantum Interferences

Cited by 190 publications

References 18 publications

Attosecond vacuum UV coherent control of molecular dynamics

Attosecond vacuum UV coherent control of molecular dynamics

Complex States of Simple Molecular Systems

Strong field quantum control by selective population of dressed states

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