Charge Oscillation Controlled Molecular Excitation

Bayer, Tim; Braun, Hendrike; Sarpe-Tudoran, C.; Siemering, R.; Hoff, P. von den; Vivie‐Riedle, Regina de; Baumert, Thomas; Wollenhaupt, M.

doi:10.1103/physrevlett.110.123003

Cited by 36 publications

(35 citation statements)

References 29 publications

Supporting

Mentioning

Contrasting

Order By: Relevance

“…In the first case, a wavepacket is launched, and its ensuing (ro-)vibrational dynamics is exploited. In the strong-field regime, the laser pulse coherently controls the dynamics during the pulse while utilizing the effective modification of the energy levels of atoms [201][202][203][204] or, respectively, the potential energy landscape experienced by the molecules, via the dynamic Stark effect [205][206][207].…”

Section: State Of the Artmentioning

confidence: 99%

Training Schrödinger’s cat: quantum optimal control

et al. 2015

View full text Add to dashboard Cite

Abstract. It is control that turns scientific knowledge into useful technology: in physics and engineering it provides a systematic way for driving a dynamical system from a given initial state into a desired target state with minimized expenditure of energy and resources. As one of the cornerstones for enabling quantum technologies, optimal quantum control keeps evolving and expanding into areas as diverse as quantumenhanced sensing, manipulation of single spins, photons, or atoms, optical spectroscopy, photochemistry, magnetic resonance (spectroscopy as well as medical imaging), quantum information processing and quantum simulation. In this communication, state-of-the-art quantum control techniques are reviewed and put into perspective by a consortium of experts in optimal control theory and applications to spectroscopy, imaging, as well as quantum dynamics of closed and open systems. We address key challenges and sketch a roadmap for future developments. ForewordThe authors of this paper represent the QUAINT consortium, a European Coordination Action on Optimal Control of Quantum Systems, funded by the European Commission Framework Programme 7, Future Emerging Technologies FET-OPEN programme and the Virtual Facility for Quantum Control (VF-QC). This consortium has considerable expertise in optimal control theory and its applications to quantum systems, both in existing areas, such as spectroscopy and imaging, and in emerging quantum technologies, such as quantum information processing, quantum communication, quantum simulation a e-mail: fwm@lusi.uni-sb.de and quantum sensing. The list of challenges for quantum control has been gathered by a broad poll of leading researchers across the communities of general and mathematical control theory, atomic, molecular-, and chemical physics, electron and nuclear magnetic resonance spectroscopy, as well as medical imaging, quantum information, communication and simulation. 144 experts in these fields have provided feedback and specific input on the state of the art, mid-term and long-term goals. Those have been summarized in this document, which can be viewed as a perspectives paper, providing a roadmap for the future development of quantum control. Because such an endeavour can hardly ever be complete (there are many additional areas of quantum control applications, such as spintronics, nano-optomechanical technologies etc.), this roadmap

show abstract

Section: State Of the Artmentioning

confidence: 99%

Training Schrödinger’s cat: quantum optimal control

et al. 2015

View full text Add to dashboard Cite

show abstract

“…amplitude of VUV harmonics, it is possible to induce full electromagnetic transparency in He, by destructively interfering two electronic wave packets of the same amplitude and opposite phases (26). Other recent work used shaped intense femtosecond laser pulses to manipulate populations by controlling the oscillating charge distribution in a potassium dimer (27).…”

Section: Significancementioning

confidence: 99%

Attosecond vacuum UV coherent control of molecular dynamics

Ranitovic

Hogle

Rivière

et al. 2014

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

123

View full text Add to dashboard Cite

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...

show abstract

“…[25] Within that context femtosecond time-resolved photoelectron spectroscopy [26,27] has been used to study nuclear dynamics [26,28] as well as changes in the electronic structure [29] on electronically excited molecular states. Direct control of charge oscillations for molecular excitation [30] as well as the generation and detection of atomic ring currents [31] has been demonstrated. In addition, it has been shown that polarization-shaped laser pulses give access to the vectorial aspects of light-matter interaction [32] and that the momentum distribution of photoelectrons resulting from multiphoton ionization with polarization-shaped laser pulses can be crafted in a sophisticated fashion [33] and detected with the help of tomographic reconstruction methods.…”

Section: Introductionmentioning

confidence: 99%

Photoelectron Circular Dichroism of Bicyclic Ketones from Multiphoton Ionization with Femtosecond Laser Pulses

et al. 2014

Self Cite

View full text Add to dashboard Cite

Photoelectron circular dichroism (PECD) is a CD effect up to the ten-percent regime and shows contributions from higher-order Legendre polynomials when multiphoton ionization is compared to single-photon ionization. We give a full account of our experimental methodology for measuring the multiphoton PECD and derive quantitative measures that we apply on camphor, fenchone and norcamphor. Different modulations and amplitudes of the contributing Legendre polynomials are observed despite the similarity in chemical structure. In addition, we study PECD for elliptically polarized light employing tomographic reconstruction methods. Intensity studies reveal dissociative ionization as the origin of the observed PECD effect, whereas ionization of the intermediate resonance is dominating the signal. As a perspective, we suggest to make use of our tomographic data as an experimental basis for a complete photoionization experiment and give a prospect of PECD as an analytic tool.

show abstract

Charge Oscillation Controlled Molecular Excitation

Cited by 36 publications

References 29 publications

Training Schrödinger’s cat: quantum optimal control

Training Schrödinger’s cat: quantum optimal control

Attosecond vacuum UV coherent control of molecular dynamics

Photoelectron Circular Dichroism of Bicyclic Ketones from Multiphoton Ionization with Femtosecond Laser Pulses

Contact Info

Product

Resources

About