Space- and time-resolved understanding of excited states in these materials will lead to higher efficiencies


The importance of e-beam is twofold; first as a direct wafer pattering technology for lower volume production, and second as a mask writing technology for high volume projection extreme ultraviolet lithography techniques. Nanopatterning of EUV masks to achieve specific functionality is further complicated by the fact that EUV masks are comprised of complex material systems of alternating single digit nm layers of high and low-Z materials to achieve high reflectivity at EUV wavelengths. Our goal is to enable new functionalities in these structures such as increased angular bandwidth, through the development of new aperiodic coatings and a deep understanding of the optical properties of the underlying materials and interfaces. We also seek to enable new optical wavefront encoding techniques through the development of etch processes compatible with the complex multilayer structures of EUV masks.Our most significant accomplishment has been to develop a new strong phase shift mask design for EUV lithography enabling an improvement in throughput for dense contact hole printing and a relaxation in mask patterning resolution requirements. Additionally a reproducible process for the fabrication of such masks for EUV lithography has been developed. Our method uses a three component nanolayered structure. After completion of the LDRD project the developed process was used to fabricate a test mask that we are in the process of characterizing in an EUV microscope at the ALS. As part of the mask process development,vertical grow rack ebeam patterning capabilities were refined and these capabilities help lead to new gift funding by Inpria corporation expected in Feb. 2015.

The mask development process also required refinement of our nano-layered coating capabilities and characterization which led to a related contract with Applied Materials which kicked off at the end of last year. That project was focused on understanding the impact of roughness on nanolayered structures such as the phase shift mask we developed. The purpose of this project is develop new time-resolved resonant X-ray scattering approaches to advance our understanding of self-organized patterns of charge, spin, and orbital order and the rapid interactions that drive their formation in complex materials. These mesoscale patterns spawn novel states of electronic matter. The competition between such phases leads to important new physics and exotic properties such as metal-to-insulator transitions, high-TC superconductivity, and colossal magne to resistance. A key challenge in understanding and manipulating electronically ordered materials is to disentangle the cause/effect interactions that drive the formation and fluctuating evolution of these competing ordered phases. To this end, we will perturbatively excite specific material modes and track the coupled order parameters in the time domain using advanced X-ray techniques including resonant scattering, spectroscopy, and dichroism at the Advanced Light Source and at the Linac Coherent Light Source. Resonant X-ray scattering is selectively sensitive to charge, spin, and orbital order at the atomic scale. X-ray dichroism can separate spin and orbital contributions to magnetic order. Coupling between these order parameters will be revealed by their disparate time responses. The time-profile of their response will provide insight to fluctuations and glassy behavior that often arise in complex oxides. Broadband THz/mid-IR spectroscopy will reveal how charge transport and lattice vibrations are coupled to different electronic order parameters. In conjunction with resonant optical or mid-IR vibrational excitation, these experiments will allow us to shed light on the salient ultrafast interactions that govern the physics of strongly correlated materials. Our studies will focus on model complex transition-metal oxide materials, and rare-earth lanthanide metals. Our most significant accomplishment has been to demonstrate that resonant X-ray scattering is an effective probe of the Skyrmion phase in Cu2OSeO3.

The cubic insulator Cu2OSeO3 is a model system for understanding Skyrmions, which are topologically protected, particle-like excitations that emerge as a periodic array of magnetic vortices when the material symmetry is broken under the application of a modest magnetic field. Understanding the origin and dynamics of this novel phase is of tremendous interest for spintronics and related device applications. A second significant accomplishment has been the first experimental studies of spin-helix dynamics in the rare-earth lanthanide metal dysprosium. Time-resolved resonant X-ray scattering reveals the dynamic response of the helical spin order to injection of a transient unpolarized spin current. The observed spin dynamics are significantly slower than that exhibited by the ferromagnetic phase in lanthanide metals and are strongly dependent on temperature and excitation fluence. We are in the process of applying similar dynamic X-ray studies to the Cu2OSeO3 Skyrmion material. Our goal is to develop an understanding of excitons and other excited states in photoactive materials with high spatiotemporal resolution, which will lead to breakthroughs in many energy conversion technologies. For example, molecular photovoltaics are promising for solar energy conversion because they are cheap, lightweight, and flexible, and because their properties can be easily tuned via organic synthesis. However, OPVs suffer from low efficiencies.Despite more than two decades of past work, the transport and spectroscopic properties of organic materials in photovoltaics – and the nature and dynamics of their excitations – continue to be debated. A major challenge is the lack of knowledge of the interplay between morphology and excited states of these organic semiconductors. For this LDRD we had proposed to develop and combine new approaches to synthesis, theory, and spectroscopy to, for the first time, spatially map, with nm-resolution, the evolution of excitons – as a function of molecular morphology – in well-defined tailored organic materials as a function of time.

We suggested the use of state-of-the-art, materials-specific excited-state theory to interpret the exciton dynamics, study the microscopic origins of their dissociation and degradation processes, and, ultimately, predict molecular moieties and morphologies leading to robust and efficient energy conversion materials. The purpose of this project is to dramatically increase our understanding of the chemical and nuclear behavior of nuclei at the far reaches of stability by revolutionizing the techniques available to study these nuclei. Transfermium nuclei are produced in nuclear reactions between accelerated beams and rotating targets and at rates of atoms-per-second to atoms-per-year. Currently, the most advanced method for studying atomic properties of transfermium elements currently involves using aqueous phase and gas phase chemistry, which must be done on single atoms. Due to this, the current status of knowledge of atomic state energies in transfermium elements results solely from theoretical calculations with errors on the order of 0.3 eV. With this project, we will develop a more direct method for determining the behavior of the atomic orbitals using laser spectroscopic techniques to obtain high-precision measurements of energy levels of atomic transitions and ionization potentials. These techniques can measure the energies of atomic transitions to within 3×10-5 eV, four orders of magnitude better than the current calculations. Detailed knowledge of atomic transitions at this level will greatly increase our knowledge of atomic and nuclear properties of elements at the limits of stability, including energies of atomic transitions, ionization potentials,vertical grow table hyperfine structure and isotope/isomer shifts. This information will allow for the determination of nuclear spins, electromagnetic moments, the change of the nuclear mean square charge radii and chemical properties of the heaviest nuclei.Our most significant accomplishment has been to design a system suitable for studying transfermium nuclei at LBNL. One of the main challenges with developing laser spectroscopy systems for rare nuclei are the expected low efficiencies of <1% for excitation and detection of the nuclei. As such, we have focused on increasing production and efficiency throughout the design. We have developed a new target design that will allow for bombarding the targets with particle-microamp beam intensities – a factor of four increase over current levels. The new targets are currently being produced and will be tested during a beamtime in February 2015. We have developed a gas chamber to mate to the exit of the pre-existing Berkeley Gas-filled Separator , an instrument that is used to separate transfermium nuclei from the beam and unwanted reaction products. This gas chamber will slow the transfermium nuclei down from 40- 50 MeV to thermal velocities with high efficiency. As transfermium nuclei tend to be ionized when they slow down, we have also designed system to attract the ions to a well-defined volume where they can be neutralized, before re-ionization with a two-step resonance-ionization technique. We are in the process of commissioning the gas catcher and finalizing the design of the neutralization and re-ionization chamber. The purpose of this project is to better understand the conditions leading to the creation of the elements in extreme astrophysical environments. Our approach is to use advanced simulation codes on high performance computing systems to model the dynamics, nucleosynthesis, and the radiative transport of supernova explosions and neutron star mergers. Our end-to-end calculations will allow us to predict the composition, energy and geometry of the ejecta, and thereby derive signatures that are directly comparable to observational data.

In this way, we will improve our understanding of the physical conditions in explosive astrophysical environments, identify indicators of novel nuclear physics occurring within them, and help clarify the origin of the heavy elements in the Universe. We simulate the dynamics and radiation transport of explosions using a variety of codes run on modern supercomputers. The smoothed particle hydrodynamics code SNSPH is used to model the dynamics of compact object mergers. In addition, we use the grid based adaptive mesh refinement hydrodynamics code CASTRO to model detonations. The radiation transport problems is addressed using the SEDONA code, an implicit Monte Carlo transport code which includes modern acceleration and variation reduction techniques, along with our newly developed MC code SEDONA-BOX. Our primary computational accomplishment has been the development of a new MC code that uses the BoxLib framework of CASTRO provide a domain decomposed grid. This code permits radiative transfer calculations to be carried out with orders of magnitude better resolution then has been the standard in the field. Our primary research accomplishments have focused on two different classes of astrophysical explosions: thermonuclear supernovae arising from the merger of two white dwarfs, and radioactive transients from the merger of two neutron stars. Our studies of white dwarf mergers demonstrated that this channel can reproduce observations of a diverse range of thermonuclear supernovae, from those of normal brightness to the most extreme luminosity events. The models also displayed a width-luminosity relation similar to the empirical relation used to calibrate thermonuclear supernovae as standardized candles for cosmology. Our studies of neutron star mergers clarified the dynamics, nucleosynthesis and radioactively powered transients resulting from these events. We found that heavy elements could be produced and ejected by tidal stripping in the merger itself, as well as in disk winds produced following the merger. We found that the ejected material underwent rapid neutron capture to a degree that depended on the neutrino flux, neutron star lifetime, and black hole spin. We demonstrated how observing the colors of the resulting radioactive transients can allow one to quantify the mass and composition of the ejected debris, thereby illuminating the cosmic origin of heavy elements like gold, platinum, and uranium. The aim of this LDRD proposal is the exploration of new approaches to detector readout and online data processing, for hadron collider physics experiments with high-intensity beams. We base this study on the ALICE experiment at the Large Hadron Collider at CERN, which will generate an unprecedented raw data rate of 1.1 Terabyte/second following a major upgrade during the LHC Long Shutdown 2 in 2018. Such data rates require qualitatively new approaches to detector readout and online processing, to ensure that all physics of interest is recorded for offline analysis with realistically achievable offline computing resources. Our specific focus is the future ALICE Inner Tracking System upgrade. However, this work is to establish a novel strategy for collision data processing that can be applied to any future high rate collider detectors. In the planned approach the paradigm of a standard eventbased reconstruction is replaced by a time-stamp driven analysis of the detector signals providing efficient, physics-ready information on the trajectories of the particles produced in the hadron/heavy-ion collisions. As part of this R&D effort we will establish physics-based requirements for ITS readout performance, based on a candidate set of observables of heavy flavor production in proton-proton and heavy ion collisions in ALICE. We will explore hardware architectures and software algorithms for both efficient data compression and data selection in silicon-based tracking detectors, guided by the physics requirements.