Toward strong field mode-selective chemistry

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

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

An optically driven quantum dot quantum computer

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

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

A terahertz half-cycle pulse was used to retrieve information stored as quantum phase in an $N$-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

Quantum Holographic Encoding in a Two-dimensional Electron Gas

The advent of bottom-up atomic manipulation heralded a new horizon for attainable information density, as it allowed a bit of information to be represented by a single atom. The discrete spacing between atoms in condensed matter has thus set a rigid limit on the maximum possible information density. While modern technologies are still far from this scale, all theoretical downscaling of devices terminates at this spatial limit. Here, however, we break this barrier with electronic quantum encoding scaled to subatomic densities. We use atomic manipulation to first construct open nanostructures--"molecular holograms"--which in turn concentrate information into a medium free of lattice constraints: the quantum states of a two-dimensional degenerate Fermi gas of electrons. The information embedded in the holograms is transcoded at even smaller length scales into an atomically uniform area of a copper surface, where it is densely projected into both two spatial degrees of freedom and a third holographic dimension mapped to energy. In analogy to optical volume holography, this requires precise amplitude and phase engineering of electron wavefunctions to assemble pages of information volumetrically. This data is read out by mapping the energy-resolved electron density of states with a scanning tunnelling microscope. As the projection and readout are both extremely near-field, and because we use native quantum states rather than an external beam, we are not limited by lensing or collimation and can create electronically projected objects with features as small as ~0.3 nm. These techniques reach unprecedented densities exceeding 20 bits/nm2 and place tens of bits into a single fermionic state.Comment: Published online 25 January 2009 in Nature Nanotechnology; 12 page manuscript (including 4 figures) + 2 page supplement (including 1 figure); supplementary movie available at http://mota.stanford.ed

Supporting technologies for a long-pulse spallation source

This is the final report of a two-year, Laboratory Directed Research and Development (LDRD) project at the Los Alamos National Laboratory (LANL). The project is directed toward the development of the technologies required for a long-pulse, spallation neutron source (LPSS). Traditionally, spallation neutron sources have used proton accelerators that provide intense, short ({le} 1{micro}s) pulses of high-energy protons to a spallation target. A LPSS uses a proton pulse with longer time duration ({approx} 1 ms) and offers the possibility of achieving very high spallation neutron fluxes at substantially lower cost. The performance of a LPSS is very dependent on the neutronic performance of the target-moderator system. A detailed study of this performance has been carried out using Monte Carlo simulations. It should be noted that a LPSS is optimally suited to a fully coupled moderator. Neutron production per proton from such a moderator is a factor of five to seven greater than that produce d by moderators used at short pulse sources. The results of these efforts have been published in a series of articles

Momentum state engineering and control in Bose-Einstein condensates

We demonstrate theoretically the use of genetic learning algorithms to coherently control the dynamics of a Bose-Einstein condensate. We consider specifically the situation of a condensate in an optical lattice formed by two counterpropagating laser beams. The frequency detuning between the lasers acts as a control parameter that can be used to precisely manipulate the condensate even in the presence of a significant mean-field energy. We illustrate this procedure in the coherent acceleration of a condensate and in the preparation of a superposition of prescribed relative phase.Comment: 9 pages incl. 6 PostScript figures (.eps), LaTeX using RevTeX, submitted to Phys. Rev. A, incl. small modifications, some references adde

Spectroscopic and Structural Probing of Excited-State Molecular Dynamics with Time-Resolved Photoelectron Spectroscopy and Ultrafast Electron Diffraction

Pump-probe measurements aim to capture the motion of electrons and nuclei on their natural timescales (femtoseconds to attoseconds) as chemical and physical transformations take place, effectively making molecular movies with short light pulses. However, the quantum dynamics of interest are filtered by the coordinate-dependent matrix elements of the chosen experimental observable. Thus, it is only through a combination of experimental measurements and theoretical calculations that one can gain insight into the internal dynamics. Here, we report on a combination of structural (relativistic ultrafast electron diffraction, or UED) and spectroscopic (time-resolved photoelectron spectroscopy, or TRPES) measurements to follow the coupled electronic and nuclear dynamics involved in the internal conversion and photodissociation of the polyatomic molecule, diiodomethane (CH2I2). While UED directly probes the 3D nuclear dynamics, TRPES only serves as an indirect probe of nuclear dynamics via Franck-Condon factors, but it is sensitive to electronic energies and configurations, via Koopmans\u27 correlations and photoelectron angular distributions. These two measurements are interpreted with trajectory surface hopping calculations, which are capable of simulating the observables for both measurements from the same dynamics calculations. The measurements highlight the nonlocal dynamics captured by different groups of trajectories in the calculations. For the first time, both UED and TRPES are combined with theory capable of calculating the observables in both cases, yielding a direct view of the structural and nonadiabatic dynamics involved

PhD TUTORIAL: Using feedback for coherent control of quantum systems

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

Optimized Dynamical Decoupling in a Model Quantum Memory

We present experimental measurements on a model quantum system that demonstrate our ability to dramatically suppress qubit error rates by the application of optimized dynamical decoupling pulse sequences in a variety of experimentally relevant noise environments. We provide the first demonstration of an analytically derived pulse sequence developed by Uhrig, and find novel sequences through active, real-time experimental feedback. These new sequences are specially tailored to maximize error suppression without the need for a priori knowledge of the ambient noise environment. We compare these sequences against the Uhrig sequence, and the well established CPMG-style spin echo, demonstrating that our locally optimized pulse sequences outperform all others under test. Numerical simulations show that our locally optimized pulse sequences are capable of suppressing errors by orders of magnitude over other existing sequences. Our work includes the extension of a treatment to predict qubit decoherence under realistic conditions, including the use of finite-duration, square $\pi$ pulses, yielding strong agreement between experimental data and theory for arbitrary pulse sequences. These results demonstrate the robustness of qubit memory error suppression through dynamical decoupling techniques across a variety of qubit technologies.Comment: Subject to press embarg