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Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angstrom spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 angstrom) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.
We present results on ultrafast gas electron diffraction (UGED) experiments with femtosecond resolution using the MeV electron gun at SLAC National Accelerator Laboratory. UGED is a promising method to investigate molecular dynamics in the gas phase because electron pulses can probe the structure with a high spatial resolution. Until recently, however, it was not possible for UGED to reach the relevant timescale for the motion of the nuclei during a molecular reaction. Using MeV electron pulses has allowed us to overcome the main challenges in reaching femtosecond resolution, namely delivering short electron pulses on a gas target, overcoming the effect of velocity mismatch between pump laser pulses and the probe electron pulses, and maintaining a low timing jitter. At electron kinetic energies above 3 MeV, the velocity mismatch between laser and electron pulses becomes negligible. The relativistic electrons are also less susceptible to temporal broadening due to the Coulomb force. One of the challenges of diffraction with relativistic electrons is that the small de Broglie wavelength results in very small diffraction angles. In this paper we describe the new setup and its characterization, including capturing static diffraction patterns of molecules in the gas phase, finding time-zero with sub-picosecond accuracy and first time-resolved diffraction experiments. The new device can achieve a temporal resolution of 100 fs root-mean-square, and sub-angstrom spatial resolution. The collimation of the beam is sufficient to measure the diffraction pattern, and the transverse coherence is on the order of 2 nm. Currently, the temporal resolution is limited both by the pulse duration of the electron pulse on target and by the timing jitter, while the spatial resolution is limited by the average electron beam current and the signal-to-noise ratio of the detection system. We also discuss plans for improving both the temporal resolution and the spatial resolution.
The Atlantic meridional overturning circulation (AMOC)—a system of ocean currents in the North Atlantic—has a major impact on climate, yet its evolution during the industrial era is poorly known owing to a lack of direct current measurements. Here we provide evidence for a weakening of the AMOC by about 3 ± 1 sverdrups (around 15 per cent) since the mid-twentieth century. This weakening is revealed by a characteristic spatial and seasonal sea-surface temperature ‘fingerprint’—consisting of a pattern of cooling in the subpolar Atlantic Ocean and warming in the Gulf Stream region—and is calibrated through an ensemble of model simulations from the CMIP5 project. We find this fingerprint both in a high-resolution climate model in response to increasing atmospheric carbon dioxide concentrations, and in the temperature trends observed since the late nineteenth century. The pattern can be explained by a slowdown in the AMOC and reduced northward heat transport, as well as an associated northward shift of the Gulf Stream. Comparisons with recent direct measurements from the RAPID project and several other studies provide a consistent depiction of record-low AMOC values in recent years.
Greenland ice sheet model parameters constrained using simulations of the Eemian Interglacial
(2011)
Using a new approach to force an ice sheet model, we performed an ensemble of simulations of the Greenland Ice Sheet evolution during the last two glacial cycles, with emphasis on the Eemian Interglacial. This ensemble was generated by perturbing four key parameters in the coupled regional climate-ice sheet model and by introducing additional uncertainty in the prescribed "background" climate change. The sensitivity of the surface melt model to climate change was determined to be the dominant driver of ice sheet instability, as reflected by simulated ice sheet loss during the Eemian Interglacial period. To eliminate unrealistic parameter combinations, constraints from present-day and paleo information were applied. The constraints include (i) the diagnosed present-day surface mass balance partition between surface melting and ice discharge at the margin, (ii) the modeled present-day elevation at GRIP; and (iii) the modeled elevation reduction at GRIP during the Eemian. Using these three constraints, a total of 360 simulations with 90 different model realizations were filtered down to 46 simulations and 20 model realizations considered valid. The paleo constraint eliminated more sensitive melt parameter values, in agreement with the surface mass balance partition assumption. The constrained simulations resulted in a range of Eemian ice loss of 0.4-4.4m sea level equivalent, with a more likely range of about 3.7-4.4m sea level if the GRIP delta O-18 isotope record can be considered an accurate proxy for the precipitation-weighted annual mean temperatures.
Global mean sea level has been steadily rising over the last century, is projected to increase by the end of this century, and will continue to rise beyond the year 2100 unless the current global mean temperature trend is reversed. Inertia in the climate and global carbon system, however, causes the global mean temperature to decline slowly even after greenhouse gas emissions have ceased, raising the question of how much sea-level commitment is expected for different levels of global mean temperature increase above preindustrial levels. Although sea-level rise over the last century has been dominated by ocean warming and loss of glaciers, the sensitivity suggested from records of past sea levels indicates important contributions should also be expected from the Greenland and Antarctic Ice Sheets. Uncertainties in the paleo-reconstructions, however, necessitate additional strategies to better constrain the sea-level commitment. Here we combine paleo-evidence with simulations from physical models to estimate the future sea-level commitment on a multimillennial time scale and compute associated regional sea-level patterns. Oceanic thermal expansion and the Antarctic Ice Sheet contribute quasi-linearly, with 0.4 m degrees C-1 and 1.2 m degrees C-1 of warming, respectively. The saturation of the contribution from glaciers is overcompensated by the nonlinear response of the Greenland Ice Sheet. As a consequence we are committed to a sea-level rise of approximately 2.3 m degrees C-1 within the next 2,000 y. Considering the lifetime of anthropogenic greenhouse gases, this imposes the need for fundamental adaptation strategies on multicentennial time scales.
Understanding the geologic evolution of Northern Tibetan Plateau with multiple thermochronometers
(2018)
The early onset of deformation following the India-Asia collision, Neogene expanse of uplift, and complex systems that comprise strike-slip faults, thrust faults, and intermontane basins characterize the Cenozoic tectonism of Northern Tibetan Plateau and raise two prominent questions in orogenic geodynamics: 1) What mechanism(s) control(s) the transfer of stress related to the India-Asia collision across the distance of >2000 km; and 2) Why the development of high topography was delayed in the Northern Tibetan Plateau and what does it reveal about how the internal forces and external boundary conditions evolved. To address these two questions, we reconstruct a holistic spatial-temporal deformation history of the Northern Tibetan Plateau by using a range of thermochronometers, with closure temperature spanning from 350 degrees C to-60-70 degrees C. This multi-thermochronometer study reveals three stages of faulting related cooling, in the early Cretaceous, in Paleocene-Eocene and in middle-late Miocene. We observe that Paleocene-Eocene deformation was spatially restricted and mostly occurred on reactivated Cretaceous structures, indicating a control of pre-existing weakness on early Cenozoic deformation. Extensive Neogene deformation contrasts with restricted Paleocene-Eocene deformation and relatively quiescent shortening during the Oligocene-early Miocene, which implies a change in the regional tectonics regime. Global plate reconstructions show that this tectonic reorganization is coeval with an increase in Pacific-Asia plate convergence rates. We argue that this change in regional tectonics is a result of increasing constrictive environment of the eastern plate boundary, which changed the behavior of the Altyn Tagh fault the boundary fault of Northern Tibetan Plateau, causing it to change from feeding slip into structures out of the plateau to feeding slip into structures at plateau margins.