84 research outputs found

    Toward strong field mode-selective chemistry

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    We demonstrate a new method for coherent control of bond excitation in the strong field regime. We can selectively excite one or more Raman-active modes in a molecular liquid without the need for externally generated coherent sources separated by the Stokes frequency. The method employs excitation with an intense, ultrafast, shaped pulse in a learning control loop. © 2000 American Institute of Physics.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/87467/2/613_1.pd

    Coherent control using adaptive learning algorithms

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    We have constructed an automated learning apparatus to control quantum systems. By directing intense shaped ultrafast laser pulses into a variety of samples and using a measurement of the system as a feedback signal, we are able to reshape the laser pulses to direct the system into a desired state. The feedback signal is the input to an adaptive learning algorithm. This algorithm programs a computer-controlled, acousto-optic modulator pulse shaper. The learning algorithm generates new shaped laser pulses based on the success of previous pulses in achieving a predetermined goal.Comment: 19 pages (including 14 figures), REVTeX 3.1, updated conten

    Nonresonant control of multimode molecular wave packets at room temperature

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    Includes bibliographical references (pages 033001-4).We demonstrate the creation and measurement of shaped multimode vibrational wave packets with overtone and combination mode excitation in CCl4. Excitation of wave packets through nonresonant impulsive stimulated Raman scattering allows for coherent control of molecular vibrations without passing through an electronic resonance. This technique is therefore very general and can be implemented in a large class of molecular gases and liquids at STP, which were previously inaccessible because their resonances are in the VUV

    An optically driven quantum dot quantum computer

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    We propose a quantum computer structure based on coupled asymmetric single-electron quantum dots. Adjacent dots are strongly coupled by means of electric dipole-dipole interactions enabling rapid computation rates. Further, the asymmetric structures can be tailored for a long coherence time. The result maximizes the number of computation cycles prior to loss of coherence.Comment: 4 figure

    Beable trajectories for revealing quantum control mechanisms

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    The dynamics induced while controlling quantum systems by optimally shaped laser pulses have often been difficult to understand in detail. A method is presented for quantifying the importance of specific sequences of quantum transitions involved in the control process. The method is based on a ``beable'' formulation of quantum mechanics due to John Bell that rigorously maps the quantum evolution onto an ensemble of stochastic trajectories over a classical state space. Detailed mechanism identification is illustrated with a model 7-level system. A general procedure is presented to extract mechanism information directly from closed-loop control experiments. Application to simulated experimental data for the model system proves robust with up to 25% noise.Comment: Latex, 20 pages, 13 figure

    Quantum phase retrieval of a Rydberg wave packet using a half-cycle pulse

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    A terahertz half-cycle pulse was used to retrieve information stored as quantum phase in an NN-state Rydberg atom data register. The register was prepared as a wave packet with one state phase-reversed from the others (the "marked bit"). A half-cycle pulse then drove a significant portion of the electron probability into the flipped state via multimode interference.Comment: accepted by PR

    Controlling the shape of a quantum wavefunction

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    The ability to control the shape and motion of quantum states(1,2) may lead to methods for bond-selective chemistry and novel quantum technologies, such as quantum computing. The classical coherence of laser light has been used to guide quantum systems into desired target states through interfering pathways(3-5). These experiments used the control of target properties-such as fluorescence from a dye solution(6), the current in a semiconductor(7,8) 8 Or the dissociation fraction of an excited molecule(9)-to infer control over the quantum state. Here we report a direct approach to coherent quantum control that allows us to actively manipulate the shape of an atomic electron's radial wavefunction, We use a computer-controlled laser to excite a coherent state in atomic caesium. The shape of the wavefunction is then measured(10) and the information fed back into the laser control system, which reprograms the optical field. The process is iterated until the measured shape of the wavefunction matches that of a target wavepacket, established at the start of the experiment. We find that, using a variation of quantum holography(11) to reconstruct the measured wavefunction, the quantum state can be reshaped to match the target within two iterations of the feedback loop.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/62625/1/397233a0.pd

    PhD TUTORIAL: Using feedback for coherent control of quantum systems

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    A longstanding goal in chemical physics has been the control of atoms and molecules using coherent light fields. This paper provides a brief overview of the field and discusses experiments that use a programmable pulse shaper to control the quantum state of electronic wavepackets in Rydberg atoms and electronic and nuclear dynamics in molecular liquids. The shape of Rydberg wavepackets was controlled by using tailored ultrafast pulses to excite a beam of caesium atoms. The quantum state of these atoms was measured using holographic techniques borrowed from optics. The experiments with molecular liquids involved the construction of an automated learning machine. A genetic algorithm directed the choice of shaped pulses which interacted with the molecular system inside a learning control loop. Analysis of successful pulse shapes that were found by using the genetic algorithm yield insight into the systems being controlled.Peer Reviewedhttp://deepblue.lib.umich.edu/bitstream/2027.42/48860/2/ob23r1.pd
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