A Discrete Four Stroke Quantum Heat Engine Exploring the Origin of Friction

The optimal power performance of a first principle quantum heat engine model shows friction-like phenomena when the internal fluid Hamiltonian does not commute with the external control field. The model is based on interacting two-level-systems where the external magnetic field serves as a control variable.Comment: 4 pages 3 figure

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

On the temperature dependence of the interaction-induced entanglement

Both direct and indirect weak nonresonant interactions are shown to produce entanglement between two initially disentangled systems prepared as a tensor product of thermal states, provided the initial temperature is sufficiently low. Entanglement is determined by the Peres-Horodeckii criterion, which establishes that a composite state is entangled if its partial transpose is not positive. If the initial temperature of the thermal states is higher than an upper critical value $T_{uc}$ the minimal eigenvalue of the partially transposed density matrix of the composite state remains positive in the course of the evolution. If the initial temperature of the thermal states is lower than a lower critical value $T_{lc}\leq T_{uc}$ the minimal eigenvalue of the partially transposed density matrix of the composite state becomes negative which means that entanglement develops. We calculate the lower bound $T_{lb}$ for $T_{lc}$ and show that the negativity of the composite state is negligibly small in the interval $T_{lb}<T<T_{uc}$. Therefore the lower bound temperature $T_{lb}$ can be considered as \textit{the} critical temperature for the generation of entanglement.Comment: 27 pages and 7 figure

Optimal control theory for unitary transformations

The dynamics of a quantum system driven by an external field is well described by a unitary transformation generated by a time dependent Hamiltonian. The inverse problem of finding the field that generates a specific unitary transformation is the subject of study. The unitary transformation which can represent an algorithm in a quantum computation is imposed on a subset of quantum states embedded in a larger Hilbert space. Optimal control theory (OCT) is used to solve the inversion problem irrespective of the initial input state. A unified formalism, based on the Krotov method is developed leading to a new scheme. The schemes are compared for the inversion of a two-qubit Fourier transform using as registers the vibrational levels of the $X^1\Sigma^+_g$ electronic state of Na$_2$. Raman-like transitions through the $A^1\Sigma^+_u$ electronic state induce the transitions. Light fields are found that are able to implement the Fourier transform within a picosecond time scale. Such fields can be obtained by pulse-shaping techniques of a femtosecond pulse. Out of the schemes studied the square modulus scheme converges fastest. A study of the implementation of the $Q$ qubit Fourier transform in the Na$_2$ molecule was carried out for up to 5 qubits. The classical computation effort required to obtain the algorithm with a given fidelity is estimated to scale exponentially with the number of levels. The observed moderate scaling of the pulse intensity with the number of qubits in the transformation is rationalized.Comment: 32 pages, 6 figure

Theoretical Investigation of Laser Induced Desorption of Small Molecules from Oxide Surfaces: A First Principles Study

State resolved laser induced desorption of NO molecules from a NiO(100) surface is studied theoretically. A full potential energy surface for the excited state was constructed by means of ab initio cluster calculations in addition to the potential energy surface for the ground state. Multidimensional wave packet calculations on these two surfaces allow a detailed simulation of experimental observables, such as velocity distributions and desorption probabilities, on a full ab initio basis

Density-Dependent Liquid Nitromethane Decomposition: Molecular Dynamics Simulations Based on ReaxFF

The decomposition mechanism of hot liquid nitromethane at various compressions was studied using reactive force field (ReaxFF) molecular dynamics simulations. A competition between two different initial thermal decomposition schemes is observed, depending on compression. At low densities, unimolecular C–N bond cleavage is the dominant route, producing CH_3 and NO_2 fragments. As density and pressure rise approaching the Chapman–Jouget detonation conditions (~30% compression, >2500 K) the dominant mechanism switches to the formation of the CH_(3)NO fragment via H-transfer and/or N–O bond rupture. The change in the decomposition mechanism of hot liquid NM leads to a different kinetic and energetic behavior, as well as products distribution. The calculated density dependence of the enthalpy change correlates with the change in initial decomposition reaction mechanism. It can be used as a convenient and useful global parameter for the detection of reaction dynamics. Atomic averaged local diffusion coefficients are shown to be sensitive to the reactions dynamics, and can be used to distinguish between time periods where chemical reactions occur and diffusion-dominated, nonreactive time periods

Three-Dimensional Ab Initio Quantum Dynamics of the Photodesorption of CO from Cr₂O₃(0001): Stereodynamic Effects

Having performed the first three-dimensional ab initio quantum dynamical study of photodesorption from solid surfaces, we gained mechanistic understanding of the rotational alignment observed in the CO/Cr2O3(0001) system. Our study is based on potential energy surfaces obtained by embedded cluster calculations for both the electronic ground and excited state of the adsorbate substrate complex. Stochastic wave packet calculations demonstrate the importance of the angular degrees of freedom for the microscopic picture of the desorption process in addition to the desorption coordinate

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