Molecular Quantum Computing by an Optimal Control Algorithm for Unitary Transformations

Quantum computation is based on implementing selected unitary transformations which represent algorithms. A generalized optimal control theory is used to find the driving field that generates a prespecified unitary transformation. The approach is illustrated in the implementation of one and two qubits gates in model molecular systems.Comment: 10 pages, 2 figure

Foundations for Cooperating with Control Noise in the Manipulation of Quantum Dynamics

This paper develops the theoretical foundations for the ability of a control field to cooperate with noise in the manipulation of quantum dynamics. The noise enters as run-to-run variations in the control amplitudes, phases and frequencies with the observation being an ensemble average over many runs as is commonly done in the laboratory. Weak field perturbation theory is developed to show that noise in the amplitude and frequency components of the control field can enhance the process of population transfer in a multilevel ladder system. The analytical results in this paper support the point that under suitable conditions an optimal field can cooperate with noise to improve the control outcome.Comment: submitted to Phys. Rev.

Analytical solution of the optimal laser control problem in two-level systems

The optimal control of two-level systems by time-dependent laser fields is studied using a variational theory. We obtain, for the first time, general analytical expressions for the optimal pulse shapes leading to global maximization or minimization of different physical quantities. We present solutions which reproduce and improve previous numerical results.Comment: 12 pages, 2 figure

Deterministic spatio-temporal control of nano-optical fields in optical antennas and nano transmission lines

We show that pulse shaping techniques can be applied to tailor the ultrafast temporal response of the strongly confined and enhanced optical near fields in the feed gap of resonant optical antennas (ROAs). Using finite-difference time-domain (FDTD) simulations followed by Fourier transformation, we obtain the impulse response of a nano structure in the frequency domain, which allows obtaining its temporal response to any arbitrary pulse shape. We apply the method to achieve deterministic optimal temporal field compression in ROAs with reduced symmetry and in a two-wire transmission line connected to a symmetric dipole antenna. The method described here will be of importance for experiments involving coherent control of field propagation in nanophotonic structures and of light-induced processes in nanometer scale volumes.Comment: 5 pages, 5 figure

Nine years of comparative effectiveness research education and training: initiative supported by the PhRMA Foundation

The term comparative effectiveness research (CER) took center stage with passage of the American Recovery and Reinvestment Act (2009). The companion US$1.1 billion in funding prompted the launch of initiatives to train the scientific workforce capable of conducting and using CER. Passage of the Patient Protection and Affordable Care Act (2010) focused these initiatives on patients, coining the term ‘patient-centered outcomes research’ (PCOR). Educational and training initiatives were soon launched. This report describes the initiative of the Pharmaceutical Research and Manufacturers Association of America (PhRMA) Foundation. Through provision of grant funding to six academic Centers of Excellence, to spearheading and sponsoring three national conferences, the PhRMA Foundation has made significant contributions to creation of the scientific workforce that conducts and uses CER/PCOR

Coherent control for the spherical symmetric box potential in short and intensive XUV laser fields

Coherent control calculations are presented for a spherically symmetric box potential for non-resonant two photon transition probabilities. With the help of a genetic algorithm (GA) the population of the excited states are maximized and minimized. The external driving field is a superposition of three intensive extreme ultraviolet (XUV) linearly polarized laser pulses with different frequencies in the femtosecond duration range. We solved the quantum mechanical problem within the dipole approximation. Our investigation clearly shows that the dynamics of the electron current has a strong correlation with the optimized and neutralizing pulse shape.Comment: 11 Pages 3 Figure

Electronic Coherence Dephasing in Excitonic Molecular Complexes: Role of Markov and Secular Approximations

We compare four different types of equations of motion for reduced density matrix of a system of molecular excitons interacting with thermodynamic bath. All four equations are of second order in the linear system-bath interaction Hamiltonian, with different approximations applied in their derivation. In particular we compare time-nonlocal equations obtained from so-called Nakajima-Zwanzig identity and the time-local equations resulting from the partial ordering prescription of the cummulant expansion. In each of these equations we alternatively apply secular approximation to decouple population and coherence dynamics from each other. We focus on the dynamics of intraband electronic coherences of the excitonic system which can be traced by coherent two-dimensional spectroscopy. We discuss the applicability of the four relaxation theories to simulations of population and coherence dynamics, and identify features of the two-dimensional coherent spectrum that allow us to distinguish time-nonlocal effects.Comment: 14 pages, 8 figure

Vectorial Control of Magnetization by Light

Coherent light-matter interactions have recently extended their applications to the ultrafast control of magnetization in solids. An important but unrealized technique is the manipulation of magnetization vector motion to make it follow an arbitrarily designed multi-dimensional trajectory. Furthermore, for its realization, the phase and amplitude of degenerate modes need to be steered independently. A promising method is to employ Raman-type nonlinear optical processes induced by femtosecond laser pulses, where magnetic oscillations are induced impulsively with a controlled initial phase and an azimuthal angle that follows well defined selection rules determined by the materials' symmetries. Here, we emphasize the fact that temporal variation of the polarization angle of the laser pulses enables us to distinguish between the two degenerate modes. A full manipulation of two-dimensional magnetic oscillations is demonstrated in antiferromagnetic NiO by employing a pair of polarization-twisted optical pulses. These results have lead to a new concept of vectorial control of magnetization by light

Coherent strong-field control of multiple states by a single chirped femtosecond laser pulse

We present a joint experimental and theoretical study on strong-field photo-ionization of sodium atoms using chirped femtosecond laser pulses. By tuning the chirp parameter, selectivity among the population in the highly excited states 5p, 6p, 7p and 5f, 6f is achieved. Different excitation pathways enabling control are identified by simultaneous ionization and measurement of photoelectron angular distributions employing the velocity map imaging technique. Free electron wave packets at an energy of around 1 eV are observed. These photoelectrons originate from two channels. The predominant 2+1+1 Resonance Enhanced Multi-Photon Ionization (REMPI) proceeds via the strongly driven two-photon transition $4s\leftarrow\leftarrow3s$, and subsequent ionization from the states 5p, 6p and 7p whereas the second pathway involves 3+1 REMPI via the states 5f and 6f. In addition, electron wave packets from two-photon ionization of the non-resonant transiently populated state 3p are observed close to the ionization threshold. A mainly qualitative five-state model for the predominant excitation channel is studied theoretically to provide insights into the physical mechanisms at play. Our analysis shows that by tuning the chirp parameter the dynamics is effectively controlled by dynamic Stark-shifts and level crossings. In particular, we show that under the experimental conditions the passage through an uncommon three-state "bow-tie" level crossing allows the preparation of coherent superposition states