Generation of polarization-shaped ultraviolet femtosecond pulses

Selle, Reimer; Nuernberger, Patrick; Langhojer, Florian; Dimler, Frank; Fechner, Susanne; Gerber, G.; Brixner, Tobias

doi:10.1364/ol.33.000803

Cited by 31 publications

(15 citation statements)

References 3 publications

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“…First, a bound on the time duration of an arbitrary transformation is obtained in the limit of vanishing noise, equation (12). Next, a lower bound on the purity loss rate for the evolving state in the presence of weak noise is calculated, assuming the purity loss is small in this case, equation (14). For weak noise the two bounds can be combined to obtain a lower bound on the purity loss during the transformation, equation (15).…”

Section: Purity and Fidelitymentioning

confidence: 99%

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Quantum control with noisy fields: computational complexity versus sensitivity to noise

2014

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A closed quantum system is defined as completely controllable if an arbitrary unitary transformation can be executed using the available controls. In practice, control fields are a source of unavoidable noise, which has to be suppressed to retain controllability. Can one design control fields such that the effect of noise is negligible on the time-scale of the transformation? This question is intimately related to the fundamental problem of a connection between the computational complexity of the control problem and the sensitivity of the controlled system to noise. The present study considers a paradigm of control, where the Lie-algebraic structure of the control Hamiltonian is fixed, while the size of the system increases with the dimension of the Hilbert space representation of the algebra. We find two types of control tasks, easy and hard. Easy tasks are characterized by a small variance of the evolving state with respect to the operators of the control operators. They are relatively immune to noise and the control field is easy to find. Hard tasks have a large variance, are sensitive to noise and the control field is hard to find. The influence of noise increases with the size of the system, which

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Section: Purity and Fidelitymentioning

confidence: 99%

“…Experimentally, there has been remarkable success in constructing devices designed to generate arbitrary control fields [12][13][14]. Nevertheless, in practice controllability is hard to achieve even for small quantum systems [15][16][17].…”

Section: Introductionmentioning

confidence: 99%

Quantum control with noisy fields: computational complexity versus sensitivity to noise

2014

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“…Femtosecond pulse shaping offers many control parameters as the spectral phase and amplitude [35] or also the polarization state [36,37] can be modified at independent frequency positions. Further developments extended polarization shaping to the ultraviolet regime [38] and to combined amplitude and polarization control [39][40][41]. Recently, complete vector-field shaping with an inherently phase-stable geometry was introduced [42] now providing control over all four degrees of freedom of femtosecond light pulses independently, i.e.…”

Section: Introductionmentioning

confidence: 99%

Analytic coherent control of plasmon propagation in nanostructures

et al. 2009

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We present general analytic solutions for optical coherent control of electromagnetic energy propagation in plasmonic nanostructures. Propagating modes are excited with tightly focused ultrashort laser pulses that are shaped in amplitude, phase, and polarization (ellipticity and orientation angle). We decouple the interplay between two main mechanisms which are essential for the control of local near-fields. First, the amplitudes and the phase difference of two laser pulse polarization components are used to guide linear flux to a desired spatial position. Second, temporal compression of the near-field at the target location is achieved using the remaining free laser pulse parameter to flatten the local spectral phase. The resulting enhancement of nonlinear signals from this intuitive analytic two-step process is compared to and confirmed by the results of an iterative adaptive learning loop in which an evolutionary algorithm performs a global optimization. Thus, we gain detailed insight into why a certain complex laser pulse shape leads to a particular control target. This analytic approach may also be useful in a number of other coherent control scenarios.

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“…It should be emphasized that the initial relative phase θ of the superposed quasi-degenerate states (i.e., the initial direction of ring currents) can be controlled by the ellipticity angle β and orientation angle δ of the applied laser. Generation of polarization-shaped femtosecond UV laser pulses has become experimentally realizable [63][64][65][66]. The efficient scheme to produce circularly polarized attosecond XUV laser pulses has been theoretically proposed [67].…”

Section: Case Of Quasi-degenerate Excited Statesmentioning

confidence: 99%

Laser-Control of Ultrafast π-Electron Ring Currents in Aromatic Molecules: Roles of Molecular Symmetry and Light Polarization

2018

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Being motivated by the recent progress in attosecond laser technology, we theoretically explore the strategy of inducing ultrafast electron dynamics inherent to aromatic molecules, i.e., ring currents by means of polarized laser pulses. The main topic of discussion is how to control the direction of ring currents in an aromatic molecule of low symmetry, for which the design of an efficient control pulse cannot be achieved intuitively. We first consider a system with a single aromatic ring and show that coherent π-electron angular momentum, which oscillates with time, can be produced and controlled by a polarized laser pulse with its ellipticity and orientation properly chosen. Nonadiabatic couplings with molecular vibration gradually weaken the angular momentum, while the vibrational amplitude strongly depends on the polarization of incident light. This suggests the conversion of the polarization dependence of ring current into that of subsequent vibration, which may open a way to detect laser-driven ultrafast electron dynamics by vibrational spectroscopy. The laser-control scheme for the ring current is then extended to a molecule with two aromatic rings, which exhibits characteristic phenomena absent in that with a single ring. We demonstrate that two-dimensional switching of the direction of angular momentum is possible in such molecules. In addition, ring current can be localized at a specific ring by tailored lasers. The application of the present control method to polycyclic aromatic hydrocarbons will lead to the development of next-generation organic optical switching devices.

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Generation of polarization-shaped ultraviolet femtosecond pulses

Cited by 31 publications

References 3 publications

Quantum control with noisy fields: computational complexity versus sensitivity to noise

Quantum control with noisy fields: computational complexity versus sensitivity to noise

Analytic coherent control of plasmon propagation in nanostructures

Laser-Control of Ultrafast π-Electron Ring Currents in Aromatic Molecules: Roles of Molecular Symmetry and Light Polarization

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