Laser control for the optimal evolution of pure quantum states

Starting from an initial pure quantum state, we present a strategy for reaching a target state corresponding to the extremum (maximum or minimum) of a given observable. We show that a sequence of pulses of moderate intensity, applied at times when the average of the observable reaches its local or global extremum, constitutes a strategy transferable to different control issues. Among them, post-pulse molecular alignment and orientation are presented as examples. The robustness of such strategies with respect to experimentally relevant parameters is also examined.Comment: 16 pages, 9 figure

Reaching optimally oriented molecular states by laser kicks

We present a strategy for post-pulse orientation aiming both at efficiency and maximal duration within a rotational period. We first identify the optimally oriented states which fulfill both requirements. We show that a sequence of half-cycle pulses of moderate intensity can be devised for reaching these target states.Comment: 4 pages, 3 figure

Pulse-driven quantum dynamics beyond the impulsive regime

We review various unitary time-dependent perturbation theories and compare them formally and numerically. We show that the Kolmogorov-Arnold-Moser technique performs better owing to both the superexponential character of correction terms and the possibility to optimize the accuracy of a given level of approximation which is explored in details here. As an illustration, we consider a two-level system driven by short pulses beyond the sudden limit.Comment: 15 pages, 5 color figure

Pulse-driven near-resonant quantum adiabatic dynamics: lifting of quasi-degeneracy

We study the quantum dynamics of a two-level system driven by a pulse that starts near-resonant for small amplitudes, yielding nonadiabatic evolution, and induces an adiabatic evolution for larger amplitudes. This problem is analyzed in terms of lifting of degeneracy for rising amplitudes. It is solved exactly for the case of linear and exponential rising. Approximate solutions are given in the case of power law rising. This allows us to determine approximative formulas for the lineshape of resonant excitation by various forms of pulses such as truncated trig-pulses. We also analyze and explain the various superpositions of states that can be obtained by the Half Stark Chirped Rapid Adiabatic Passage (Half-SCRAP) process.Comment: 21 pages, 12 figure

Time-dependent unitary perturbation theory for intense laser driven molecular orientation

We apply a time-dependent perturbation theory based on unitary transformations combined with averaging techniques, on molecular orientation dynamics by ultrashort pulses. We test the validity and the accuracy of this approach on LiCl described within a rigid-rotor model and find that it is more accurate than other approximations. Furthermore, it is shown that a noticeable orientation can be achieved for experimentally standard short laser pulses of zero time average. In this case, we determine the dynamically relevant parameters by using the perturbative propagator, that is derived from this scheme, and we investigate the temperature effects on the molecular orientation dynamics.Comment: 16 pages, 6 figure

Functionalized Gold Nanoparticles with Electropolymerizable π-Conjugated Systems for a Neuro-inspired Memristive Nanoparticle Organic Synapse-Transistor

Nanoparticle Organic Memory Field-Effect Transistors (NOMFET) are molecule-based devices that exhibit the main behavior of a biological spiking synapse. This behavior is obtained by virtue of the combination of two properties of the NOMFET: the transconductance gain of the transistor and the memory effect due to the presence of nanoparticles (NPs) which are used as nanoscale capacitors to store the electrical charges, and which are embedded into an organic semiconducting layer [1]. Thus, the transconductance of the transistor can be dynamically tuned by the amount of charge in the NPs. In this context, we present here a novel method for the elaboration of NOMFET active materials based on the electrochemical deposition of gold NPs grafted with alkanethiol-terminated π-conjugated precursors combining low oxidation potential and high reactivity. The straightforward electropolymerization of these new precursors leads to the formation of a semiconducting network in which the electronic and transport properties and the charging/discharging speed of the gold NPs can be modulated. Such hybrid material could advantageously replace the pentacene layer generally used in NOMFETs. This novel approach is based on previously demonstrated enhancement of charge-tunneling across monolayers of SAMs of alkanethiol-bithiophenic systems on a planar gold surface after electrochemical conversion into more extended conjugated systems [2]. The synthesis of the precursors and nanoparticles will be described and the morphology and electronic properties of the hybrid electropolymerized films will be discussed with regard to the behavior of the resulting NOMFET-devices. [1] F. Alibart, S. Pleutin, D. Guerin, C. Novembre, S. Lenfant, K. Lmimouni, C. Gamrat, D. Vuillaume, Adv. Funct. Mater. 2010, 20, 330-337. [2] M. Oçafrain, T. K. Tran, P. Blanchard, S. Lenfant, S. Godey, D. Vuillaume, J. Roncali, Adv. Funct. Mater. 2008, 18, 2163-2171

Chiral molecules split light: Reflection and refraction in a chiral liquid

A light beam changes direction as it enters a liquid at an angle from another medium, such as air. Should the liquid contain molecules that lack mirror symmetry, then it has been predicted by Fresnel that the light beam will not only change direction, but will actually split into two separate beams with a small difference in the respective angles of refraction. Here we report the observation of this phenomenon. We also demonstrate that the angle of reflection does not equal the angle of incidence in a chiral medium. Unlike conventional optical rotation, which depends on the path-length through the sample, the reported reflection and refraction phenomena arise within a few wavelengths at the interface and thereby suggest a new approach to polarimetry that can be used in microfluidic volumes

Tribological properties of room temperature fluorinated graphite heat-treated under fluorine atmosphere

This work is concerned with the study of the tribologic properties of room temperature fluorinated graphite heat-treated under fluorine atmosphere. The fluorinated compounds all present good intrinsic friction properties (friction coefficient in the range 0.05–0.09). The tribologic performances are optimized if the materials present remaining graphitic domains (influenced by the presence of intercalated fluorinated species) whereas the perfluorinated compounds, where the fluorocarbon layers are corrugated (armchair configuration of the saturated carbon rings) present higher friction coefficients. Raman analyses reveal that the friction process induces severe changes in the materials structure especially the partial re-building of graphitic domains in the case of perfluorinated compounds which explains the improvement of μ during the friction tests for these last materials