Related papers: Optimization Schemes for Selective Molecular Cleav…
We propose a methodology to design optimal pulses for achieving quantum optimal control on molecular systems. Our approach constrains pulse shapes to linear combinations of a fixed number of experimentally relevant pulse functions. Quantum…
Combining the features of molecular wires and femtosecond laser pulses gives the unique opportunity to optically switch electron currents in molecular devices with very high speed. Based on a weak-coupling approximation between wire and…
How fast can a laser pulse ionize an atom? We address this question by considering pulses that carry a fixed time-integrated energy per-area, and finding those that achieve the double requirement of maximizing the ionization that they…
Laser cooling of molecules employing broadband optical pumping involves a timescale separation between laser excitation and spontaneous emission. Here, we optimize the optical pumping step using shaped laser pulses. We derive two…
We develop an hybrid quantum-classical algorithm to solve an optimal population transfer problem for a molecule subject to a laser pulse. The evolution of the molecular wavefunction under the laser pulse is simulated on a quantum computer,…
The lack of a direct map between control fields and desired control objectives poses a significant challenge in applying quantum control theory to quantum technologies. Here, we propose an analytical framework to precisely control a limited…
New features of molecular wires can be observed when they are irradiated by laser fields. These effects can be achieved by periodically oscillating fields but also by short laser pulses. The theoretical foundation used for these…
In this work, we extend the quantum optimal control theory of molecules subject to ultrashort laser pulses to the case of solvated systems, explicitly including the solvent dielectric properties in the system Hamiltonian. A reliable…
In this work, we investigate how and to which extent a quantum system can be driven along a prescribed path in Hilbert space by a suitably shaped laser pulse. To calculate the optimal, i.e., the variationally best pulse, a properly defined…
A new concept of the molecular structure optimization method based on quantum dynamics computations is presented. Nuclei are treated as quantum mechanical particles, as are electrons, and the many-body wave function of the system is…
We present an implementation of optimal control theory for the first-principles non-adiabatic Ehrenfest Molecular Dynamics model, which describes a condensed matter system by considering classical point-particle nuclei, and quantum…
The control of quantum dynamics via specially tailored laser pulses is a long-standing goal in physics and chemistry. Partly, this dream has come true, as sophisticated pulse shaping experiments allow to coherently control product ratios of…
Understanding and controlling the electronic as well as ro-vibrational motion and, thus, the entire chemical dynamics in molecules is the ultimate goal of ultrafast laser and imaging science. In photochemistry, laser-induced dissociation…
The possibility of achieving highly selective excitation of low metastable states of hydrogen and helium atoms by using short laser pulses with reasonable parameters is demonstrated theoretically. Interactions of atoms with the laser field…
Genetic algorithms, as implemented in optimal control strategies, are currently successfully exploited in a wide range of problems in molecular physics. In this context, laser control of molecular alignment and orientation remains a very…
We study the efficiency of modulated laser pulses to produce efficient and fast charge localization transitions in a two-electron double quantum dot. We use a configuration interaction method to calculate the electronic structure of a…
We train a model atom to recognize hand-written digits between 0 and 9, employing intense light--matter interaction as a computational resource. For training, individual images of hand-written digits in the range 0-9 are converted into…
Advances of quantum control technology have led to nearly perfect single-qubit control of nuclear spins and atomic hyperfine ground states. In contrast, quantum control of strong optical transitions, even for free atoms, are far from being…
Starting from an initial pure quantum state, we present a strategy for reaching a target state corresponding to the extremum (maximum or minimum) of a given observable. We show that a sequence of pulses of moderate intensity, applied at…
Achieving high-fidelity control of quantum systems is essential for realization of a practical quantum computer. Composite pulse sequences which suppress different types of errors can be nested to suppress a wide variety of errors but the…