A magnetic liquid deformable mirror for high stroke and low order axially symmetrical aberrations

We present a new class of magnetically shaped deformable liquid mirrors made of a magnetic liquid (ferrofluid). Deformable liquid mirrors offer advantages with respect to deformable solid mirrors: large deformations, low costs and the possibility of very large mirrors with added aberration control. They have some disadvantages (e.g. slower response time). We made and tested a deformable mirror, producing axially symmetrical wavefront aberrations by applying electric currents to 5 concentric coils made of copper wire wound on aluminum cylinders. Each of these coils generates a magnetic field which combines to deform the surface of a ferrofluid to the desired shape. We have carried out laboratory tests on a 5 cm diameter prototype mirror and demonstrated defocus as well as Seidel and Zernike spherical aberrations having amplitudes up to 20 microns, which was the limiting measurable amplitude of our equipmentComment: To appear in Optics Expres

Post-cutting Mortality Following Experimental Silvicultural Treatments in Unmanaged Boreal Forest Stands

Partial cutting has been recommended as an alternative harvesting method to ensure the sustainable management of boreal forests. The success of this approach is closely linked to the survival of residual trees as additional losses through mortality could affect post-cutting timber production at harvest. To better quantify post-cutting mortality in previously unmanaged boreal forests, we addressed two main questions: (1) what is the level of mortality 10 years after cutting? and (2) what ecological factors are involved in this phenomenon? Even-aged black spruce [Picea mariana (Mill.) B.S.P.] stands in the Canadian boreal forest were subjected to three experimental shelterwood treatments, a seed-tree treatment and an untreated control. Tree status (live/dead) was recorded prior to cutting and 10 years after cutting. Dead trees were classified as standing dead, overturned or broken. Ten years after experimental seed-tree treatment, 60% of residual trees were dead, compared to 30% for the shelterwood cuttings. Windthrow (overturned and broken trees) represented 80% of residual tree mortality; only the amount of overturning was influenced by treatment. Broken trees were associated with small-diameter trunks, stands having high growth prior to cutting, younger stands or forest plots located near to adjacent cuts (<200 m). Overturning was associated with a high harvesting intensity and large-diameter trees. Standing dead mortality was the most difficult to explain: it was related to untreated plots having suppressed and small-diameter trees. Based on these results, applying intermediate levels of harvest intensity could reduce post-cutting damage. Understanding tree mortality after cutting is essential to reduce economic losses, improve silvicultural planning and stand selection and ensure ultimately the sustainable harvest of North American boreal forests

Ring closing reaction in diarylethene captured by femtosecond electron crystallography

The photoinduced ring-closing reaction in diarylethene, which serves as a model system for understanding reactive crossings through conical intersections, was directly observed with atomic resolution using femtosecond electron diffraction. Complementary ab initio calculations were also performed. Immediately following photoexcitation, subpicosecond structural changes associated with the formation of an open-ring excited-state intermediate were resolved. The key motion is the rotation of the thiophene rings, which significantly decreases the distance between the reactive carbon atoms prior to ring closing. Subsequently, on the few picosecond time scale, localized torsional motions of the carbon atoms lead to the formation of the closed-ring photoproduct. These direct observations of the molecular motions driving an organic chemical reaction were only made possible through the development of an ultrabright electron source to capture the atomic motions within the limited number of sampling frames and the low data acquisition rate dictated by the intrinsically poor thermal conductivity and limited photoreversibility of organic materials

Femtosecond Dynamics of the Ring Closing Process of Diarylethene: A Case Study of Electrocyclic Reactions in Photochromic Single Crystals

The cyclization reaction of the photochromic diarylethene derivative 1,2-bis(2,4-dimethyl-5-phenyl-3-thienyl)perfluorocyclopentene was studied in its single crystal phase with femtosecond transient absorption spectroscopy. The transient absorption measurements were performed with a robust acquisition scheme that explicitly exploits the photoreversibility of the molecular system and monitors the reversibility conditions. The crystalline system demonstrated 3 × 104 repeatable cycles before significant degradation was observed. Immediately following photoexcitation, the excited state absorption associated with the open-ring conformation undergoes a large spectral shift with a time constant of approximately 200 fs. Following this evolution on the excited state potential energy surface, the ring closure occurs with a time constant of 5.3 ps, which is significantly slower than previously reported measurements for similar derivatives in the solution phase. Time resolved electron diffraction studies were used to further demonstrate the assignment of the transient absorption dynamics to the ring closing reaction. The mechanistic details of the ring closing are discussed in the context of prior computational work along with a vibrational mode analysis using density functional theory to give some insight into the primary motions involved in the ring closing reaction

Femtosecond Electron Diffraction and Spectroscopic Studies of a Solid State Organic Chemical Reaction

Photochromic diarylethene molecules are excellent model systems for studying electrocyclic reactions, in addition to having important technological applications in optoelectronics. The photoinduced ring-closing reaction in a crystalline photochromic diarylethene derivative was fully resolved using the complementary techniques of transient absorption spectroscopy and femtosecond electron crystallography. These studies are detailed in this thesis, together with the associated technical developments which enabled them. Importantly, the time-resolved crystallographic investigation reported here represents a highly significant proof-of-principle experiment. It constitutes the first study directly probing the molecular structural changes associated with an organic chemical reaction with sub-picosecond temporal and atomic spatial resolution -- to follow the primary motions directing chemistry.In terms of technological development, the most important advance reported is the implementation of a radio frequency rebunching system capable of producing femtosecond electron pulses of exceptional brightness. The temporal resolution of this newly developed electron source was fully characterized using laser ponderomotive scattering, confirming a 435 +/- 75 fs instrument response time with 0.20 pC bunches. The ultrafast spectroscopic and crystallographic measurements were both achieved by exploiting the photoreversibility of diarylethene. The transient absorption study was first performed, after developing a novel robust acquisition scheme for thermally irreversible reactions in the solid state. It revealed the formation of an open-ring excited state intermediate, following photoexcitation of the open-ring isomer with an ultraviolet laser pulse, with a time constant of approximately 200 fs. The actual ring closing was found to occur from this intermediate with a time constant of 5.3 +/- 0.3 ps. The femtosecond diffraction measurements were then performed using multiple crystal orientations and a large number of different samples. To analyse the results, an innovative method was developed in which the apparently complex ring-closing reaction is distilled down to a small number of basic rotations. Immediately following photoexcitation, sub-picosecond structural changes associated with the formation of the intermediate are observed. The rotation of the thiophene rings is identified as the key motion. Subsequently, on the few picosecond time scale, the time-resolved diffraction patterns are observed to converge towards those associated with the closed-ring photoproduct. The formation of the closed-ring molecule is thus unambiguously witnessed.Ph.D

Cellular orientation is guided by strain gradients

The strain-induced reorientation response of cyclically stretched cells has been well characterized in uniform strain fields. In the present study, we comprehensively analyse the behaviour of human fibroblasts subjected to a highly non-uniform strain field within a polymethylsiloxane microdevice. Our results indicate that the strain gradient amplitude and direction regulate cell reorientation through a coordinated gradient avoidance response. We provide critical evidence that strain gradient is a key physical cue that can guide cell organization. Specifically, our work suggests that cells are able to pinpoint the location under the cell of multiple physical cues and integrate this information (strain and strain gradient amplitudes and directions), resulting in a coordinated response. To gain insight into the underlying mechanosensing processes, we studied focal adhesion reorganization and the effect of modulating myosin-II contractility. The extracted focal adhesion orientation distributions are similar to those obtained for the cell bodies, and their density is increased by the presence of stretching forces. Moreover, it was found that the myosin-II activity promoter calyculin-A has little effect on the cellular response, while the inhibitor blebbistatin suppresses cell and focal adhesion alignment and reduces focal adhesion density. These results confirm that similar internal structures involved in sensing and responding to strain direction and amplitude are also key players in strain gradient mechanosensing and avoidance

'Making the molecular movie': first frames

Recent advances in high-intensity electron and X-ray pulsed sources now make it possible to directly observe atomic motions as they occur in barrier-crossing processes. These rare events require the structural dynamics to be triggered by femtosecond excitation pulses that prepare the system above the barrier or access new potential energy surfaces that drive the structural changes. In general, the sampling process modifies the system such that the structural probes should ideally have sufficient intensity to fully resolve structures near the single-shot limit for a given time point. New developments in both source intensity and temporal characterization of the pulsed sampling mode have made it possible to make so-called 'molecular movies', i.e. measure relative atomic motions faster than collisions can blur information on correlations. Strongly driven phase transitions from thermally propagated melting to optically modified potential energy surfaces leading to ballistic phase transitions and bond stiffening are given as examples of the new insights that can be gained from an atomic level perspective of structural dynamics. The most important impact will likely be made in the fields of chemistry and biology where the central unifying concept of the transition state will come under direct observation and enable a reduction of high-dimensional complex reaction surfaces to the key reactive modes, as long mastered by Mother Nature

Ring-Closing Reaction in Diarylethene Captured by Femtosecond Electron Crystallography

The photoinduced ring-closing reaction in diarylethene, which serves as a model system for understanding reactive crossings through conical intersections, was directly observed with atomic resolution using femtosecond electron diffraction. Complementary ab initio calculations were also performed. Immediately following photoexcitation, subpicosecond structural changes associated with the formation of an open-ring excited-state intermediate were resolved. The key motion is the rotation of the thiophene rings, which significantly decreases the distance between the reactive carbon atoms prior to ring closing. Subsequently, on the few picosecond time scale, localized torsional motions of the carbon atoms lead to the formation of the closed-ring photoproduct. These direct observations of the molecular motions driving an organic chemical reaction were only made possible through the development of an ultrabright electron source to capture the atomic motions within the limited number of sampling frames and the low data acquisition rate dictated by the intrinsically poor thermal conductivity and limited photoreversibility of organic materials

Le monde peut-il nourrir tout le monde ?

Deux milliards de personnes dans le monde souffrent aujourd’hui de carences alimentaires graves, dont les trois quarts sont des paysans, et plus de 800 millions d’individus sont encore sous-alimentés. Pourtant, l’agriculture mondiale n’a jamais autant produit et la production moyenne suffirait à couvrir les besoins de la planète. Ce contexte, paradoxal et préoccupant, est de plus complexe car les situations de malnutrition ne se superposent plus au simple clivage entre pays riches et pays pauvres. Pour rendre compte du fait alimentaire dans sa dimension globale et dans toute sa complexité, cet ouvrage collectif ouvre la réflexion à divers champs disciplinaires. Économistes, sociologues, anthropologues, géographes, nutritionnistes et écologues y décrivent l’alimentation comme un fait structurant des sociétés que les crises alimentaires contribuent à déstabiliser, tant au Sud qu’au Nord. Les textes explorent des voies peu empruntées et rarement rassemblées dans un même ouvrage. La mise en œuvre d’une véritable politique alimentaire y apparaît comme un des volets indispensables à la cohérence des politiques agricoles et agro-alimentaires, afin de satisfaire les besoins des quelque neuf milliards d’hommes qui pourraient peupler notre planète en 2050

Mapping molecular motions leading to charge delocalization with ultrabright electrons

Ultrafast processes can now be studied with the combined atomic spatial resolution of diffraction methods and the temporal resolution of femtosecond optical spectroscopy by using femtosecond pulses of electrons1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14 or hard X-rays15, 16, 17, 18, 19 as structural probes. However, it is challenging to apply these methods to organic materials, which have weak scattering centres, thermal lability, and poor heat conduction. These characteristics mean that the source needs to be extremely bright to enable us to obtain high-quality diffraction data before cumulative heating effects from the laser excitation either degrade the sample or mask the structural dynamics20. Here we show that a recently developed, ultrabright femtosecond electron source7, 8, 9 makes it possible to monitor the molecular motions in the organic salt (EDO-TTF)2PF6 as it undergoes its photo-induced insulator-to-metal phase transition21, 22, 23, 24. After the ultrafast laser excitation, we record time-delayed diffraction patterns that allow us to identify hundreds of Bragg reflections with which to map the structural evolution of the system. The data and supporting model calculations indicate the formation of a transient intermediate structure in the early stage of charge delocalization (less than five picoseconds), and reveal that the molecular motions driving its formation are distinct from those that, assisted by thermal relaxation, convert the system into a metallic state on the hundred-picosecond timescale. These findings establish the potential of ultrabright femtosecond electron sources7, 8, 9, 10, 11, 12, 13, 14 for probing the primary processes governing structural dynamics with atomic resolution in labile systems relevant to chemistry and biology