Electronic Energy Transfer: Localized Operator Partitioning of Electronic Energy in Composite Quantum Systems

A Hamiltonian based approach using spatially localized projection operators is introduced to give precise meaning to the chemically intuitive idea of the electronic energy on a quantum subsystem. This definition facilitates the study of electronic energy transfer in arbitrarily coupled quantum systems. In particular, the decomposition scheme can be applied to molecular components that are strongly interacting (with significant orbital overlap) as well as to isolated fragments. The result leads to the proper electronic energy at all internuclear distances, including the case of separated fragments, and reduces to the well-known Forster and Dexter results in their respective limits. Numerical calculations of coherent energy and charge transfer dynamics in simple model systems are presented and the effect of collisionally induced decoherence is examined

Decoherence Effects in Reactive Scattering

Decoherence effects on quantum and classical dynamics in reactive scattering are examined using a Caldeira-Leggett type model. Through a study of dynamics of the collinear H+H2 reaction and the transmission over simple one-dimensional barrier potentials, we show that decoherence leads to improved agreement between quantum and classical reaction and transmission probabilities, primarily by increasing the energy dispersion in a well defined way. Increased potential nonlinearity is seen to require larger decoherence in order to attain comparable quantum-classical agreement.Comment: 25 pages, 6 figures, to be published in J. Chem. Phy

Advances in decoherence control

I address the current status of dynamical decoupling techniques in terms of required control resources and feasibility. Based on recent advances in both improving the theoretical design and assessing the control performance for specific noise models, I argue that significant progress may still be possible on the road of implementing decoupling under realistic constraints.Comment: 14 pages, 3 encapsulated eps figures. To appear in Journal of Modern Optics, Special Proceedings Volume of the XXXIV Winter Colloquium on the Physics of Quantum Electronics, Snowbird, Jan 200

Cold Atomic Collisions: Coherent Control of Penning and Associative Ionization

Coherent Control techniques are computationally applied to cold (1mK < T < 1 K) and ultracold (T < 1 microK) Ne*(3s,3P2) + Ar(1S0) collisions. We show that by using various initial superpositions of the Ne*(3s,3P2) M = {-2,-1,0,1,2} Zeeman sub-levels it is possible to reduce the Penning Ionization (PI) and Associative Ionization (AI) cross sections by as much as four orders of magnitude. It is also possible to drastically change the ratio of these two processes. The results are based on combining, within the "Rotating Atom Approximation", empirical and ab-initio ionization-widths.Comment: 4 pages, 2 tables, 2 figure

Coherent Control of Quantum Chaotic Diffusion

Extensive coherent control over quantum chaotic diffusion using the kicked rotor model is demonstrated and its origin in deviations from random matrix theory is identified. Further, the extent of control in the presence of external decoherence is established. The results are relevant to both areas of quantum chaos and coherent control.Comment: 4 pages, 4 figures, to appear in Phys. Rev. Let

Aspects of quantum coherence in the optical Bloch equations

Aspects of coherence and decoherence are analyzed within the optical Bloch equations. By rewriting the analytic solution in an alternate form, we are able to emphasize a number of unusual features: (a) despite the Markovian nature of the bath, coherence at long times can be retained; (b) the long-time asymptotic degree of coherence in the system is intertwined with the asymptotic difference in level populations; (c) the traditional population-relaxation and decoherence times, $T_1$ and $T_2$, lose their meaning when the system is in the presence of an external field, and are replaced by more general overall timescales; (d) increasing the field strength, quantified by the Rabi frequency, $\Omega$, increases the rate of decoherence rather than reducing it, as one might expect; and (e) maximum asymptotic coherence is reached when the system parameters satisfy $\Omega^2 = 1/(T_1 T_2)$.Comment: 18 pages, 6 figures; to appear in J Chem Phy

Quantum Control of the Hyperfine Spin of a Cs Atom Ensemble

We demonstrate quantum control of a large spin-angular momentum associated with the F=3 hyperfine ground state of 133Cs. A combination of time dependent magnetic fields and a static tensor light shift is used to implement near-optimal controls and map a fiducial state to a broad range of target states, with yields in the range 0.8-0.9. Squeezed states are produced also by an adiabatic scheme that is more robust against errors. Universal control facilitates the encoding and manipulation of qubits and qudits in atomic ground states, and may lead to improvement of some precision measurements.Comment: 4 pages, 4 figures (color

Entanglement and Timing-Based Mechanisms in the Coherent Control of Scattering Processes

The coherent control of scattering processes is considered, with electron impact dissociation of H$_2^+$ used as an example. The physical mechanism underlying coherently controlled stationary state scattering is exposed by analyzing a control scenario that relies on previously established entanglement requirements between the scattering partners. Specifically, initial state entanglement assures that all collisions in the scattering volume yield the desirable scattering configuration. Scattering is controlled by preparing the particular internal state wave function that leads to the favored collisional configuration in the collision volume. This insight allows coherent control to be extended to the case of time-dependent scattering. Specifically, we identify reactive scattering scenarios using incident wave packets of translational motion where coherent control is operational and initial state entanglement is unnecessary. Both the stationary and time-dependent scenarios incorporate extended coherence features, making them physically distinct. From a theoretical point of view, this work represents a large step forward in the qualitative understanding of coherently controlled reactive scattering. From an experimental viewpoint, it offers an alternative to entanglement-based control schemes. However, both methods present significant challenges to existing experimental technologies

The Importance of DNA Repair in Tumor Suppression

The transition from a normal to cancerous cell requires a number of highly specific mutations that affect cell cycle regulation, apoptosis, differentiation, and many other cell functions. One hallmark of cancerous genomes is genomic instability, with mutation rates far greater than those of normal cells. In microsatellite instability (MIN tumors), these are often caused by damage to mismatch repair genes, allowing further mutation of the genome and tumor progression. These mutation rates may lie near the error catastrophe found in the quasispecies model of adaptive RNA genomes, suggesting that further increasing mutation rates will destroy cancerous genomes. However, recent results have demonstrated that DNA genomes exhibit an error threshold at mutation rates far lower than their conservative counterparts. Furthermore, while the maximum viable mutation rate in conservative systems increases indefinitely with increasing master sequence fitness, the semiconservative threshold plateaus at a relatively low value. This implies a paradox, wherein inaccessible mutation rates are found in viable tumor cells. In this paper, we address this paradox, demonstrating an isomorphism between the conservatively replicating (RNA) quasispecies model and the semiconservative (DNA) model with post-methylation DNA repair mechanisms impaired. Thus, as DNA repair becomes inactivated, the maximum viable mutation rate increases smoothly to that of a conservatively replicating system on a transformed landscape, with an upper bound that is dependent on replication rates. We postulate that inactivation of post-methylation repair mechanisms are fundamental to the progression of a tumor cell and hence these mechanisms act as a method for prevention and destruction of cancerous genomes.Comment: 7 pages, 5 figures; Approximation replaced with exact calculation; Minor error corrected; Minor changes to model syste