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Carnegie/DOE Alliance Center (CDAC): a CENTER of EXCELLENCE for HIGH PRESSURE SCIENCE and TECHNOLOGY

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Carnegie/DOE Alliance Center (CDAC): a CENTER of EXCELLENCE for HIGH PRESSURE SCIENCE and TECHNOLOGY CARNEGIE/DOE ALLIANCE CENTER A Center of Excellence for High Pressure Science and Technology Supported by the Stockpile Stewardship Academic Alliances Program of DOE/NNSA Year Three Annual Report September 2006 Russell J. Hemley, Director Ho-kwang Mao, Associate Director Stephen A. Gramsch, Coordinator Carnegie/DOE Alliance Center (CDAC): A CENTER OF EXCELLENCE FOR HIGH PRESSURE SCIENCE AND TECHNOLOGY YEAR THREE ANNUAL REPORT 1. Overview 1.1 Mission of CDAC 3 1.2 Highlights from Year 3 4 1.3 Year 3 Work Plan and Milestones 6 2. Scientific Progress 2.1 High P-T Phase Relations and Structures 10 2.2 P-V-T EOS Measurements 19 2.3 Phonons, Vibrational Thermodynamics and Elasticity 22 2.4 Plasticity, Yield Strength and Deformation 26 2.5 Electronic and Magnetic Structure and Dynamics 27 2.6 High P-T Chemistry 36 3. Education, Training, and Outreach 3.1 CDAC Graduate Students and Post-doctoral Associates 40 3.2 CDAC Collaborators 43 3.3 Undergraduate Student Participation 47 3.4 DC Area High School Outreach 49 3.5 Synergy of 21st Century High-Pressure Science and Technology Workshop 50 3.6 Visitors to CDAC 56 3.7 High Pressure Seminars 58 4. Technology Development 4.1 High P-T Experimental Techniques 60 4.2 Facilities at Brookhaven, LANSCE, and Carnegie 64 4.3 Commissioning and Activities at HPCAT 66 5. Interactions with NNSA/DP National Laboratories 5.1 Overview 67 5.2 Academic Alliance and Laboratory Collaborations 69 6. Management and Oversight 6.1 CDAC Organization and Staff 71 6.2 CDAC Oversight 73 6.3 Second Year Review 74 7. Plans for Year 4 and Beyond 7.1 Scientific and Educational Focus 75 7.2 Implementation of CDAC Phase II 75 7.3 HPCAT Upgrade 76 Appendix I CDAC Publications and Presentations for Year 3 81 Appendix II CDAC Synchrotron Users/Experiments (APS and NSLS) for Year 3 99 References 112 2 1. OVERVIEW 1.1 Mission of CDAC High P-T materials research is critical to the mission of the National Nuclear Security Administration in science-based stockpile stewardship1. The program encompasses a broad range of problems and materials – d- and f-electron elements and alloys, low-Z molecular compounds, energetic materials and detonation products, dense hydrogen, metal oxides and hydrides, and bulk materials as well as composites and interfaces. Information on these materials in crystalline, liquid, and amorphous phases and examination of phase transitions, equations of state, phonon dynamics, elasticity and plasticity, electronic and magnetic structures, and chemical reactions are essential. Moreover, addressing these problems requires the training of the next generation of scientists. The proper training of these students requires in turn their access to state-of-the-art facilities that may not be available to research groups in the NNSA Labs or in conventional academia. The Carnegie/DOE Alliance Center – CDAC – was created to support this NNSA mission. Now completing its third year, CDAC continues to address these important needs of the NNSA in scientific research and training. The success of the past year has allowed us to grow and bring a broader range of universities into the alliance. CDAC is managed by Russell J. Hemley (Director), Ho-kwang Mao (Associate Director), and Stephen Gramsch (Coordinator). CDAC consists of six formal partners together with Carnegie (the CDAC Academic Partners): Princeton University (Tom Duffy), University of Chicago (Dion Heinz), University of Illinois (Dana Dlott), University of Alabama - Birmingham (Yogesh Vohra), University of California - Berkeley (Hans-Rudolf Wenk), and California Institute of Technology (Brent Fultz). Starting with Year 4, four new academic partners have joined CDAC: New Mexico State University (Kanani Lee), Florida International University (Surendra Saxena), Texas Tech University (Yanzhang Ma), University of Nevada - Reno (Dhanesh Chandra), and Arizona State University (Jeffrey Yarger). Scientists at the National Labs (the CDAC Laboratory Partners) obtain beam time and technical training, and access to ongoing high P-T technique development at HPCAT, the dedicated high-pressure synchrotron x-ray facility at the Advanced Photon Source (APS). Laboratory scientists also take advantage of facilities at Carnegie (including NSLS). There is active cooperation with the Lujan Center in the development of high P-T neutron scattering. Finally, CDAC has an extensive list of collaborators from some 145 institutions around the world. Figure 1. Aerial photograph of the Carnegie Institution campus in Washington, D.C. where the Geophysical Laboratory is located. 3 CDAC is developing the next generation of high-pressure techniques and conducting systematic measurements of a full range of physical and chemical phenomena under extreme conditions. HPCAT, the dedicated high-pressure synchrotron x-ray facility at the Advanced Photon Source (APS) at Argonne National Laboratory is led by Ho-kwang Mao (Director) and Guoyin Shen (Project Manager). HPCAT has been developed for high pressure physics, chemistry and materials science, and is a centerpiece of the CDAC scientific program, providing technical developments and critical spectroscopic and diffraction tools. Construction of the two insertion device beamlines has been completed, and the microdiffraction station has been open to general users for nearly three years. Commissioning activities in the areas of x-ray absorption and emission, and resonant and non-resonant inelastic x-ray scattering have taken place, with this station accepting proposals from general users for approximately two years. At this point, well over 281 different users (i.e., from National Labs and academia) have conducted experiments at the facility in these two completed experimental hutches to date. Commissioning activities have been nearly completed on the two bending magnet beamlines, and these two stations will be accepting general users in the first run of 2007. The goal of four independently operating experimental hutches, a cornerstone of the initial HPCAT concept, has now been realized. High-pressure neutron facilities at LANSCE, LANL, synchrotron infrared spectroscopy at the National Synchrotron Light Source (NSLS) at Brookhaven National Laboratory (BNL), and specialized high-pressure facilities at Carnegie complement this effort. At Carnegie, there are important new developments in high P-T spectroscopy of molecular systems, high P-T cell designs, and CVD diamond growth. Experiments in high-pressure geoscience and planetary science provide valuable insight into problems in stewardship science and provide an important training ground for students and other researchers for future work in the NNSA Laboratory complex. There are also close interactions with theorists at Center institutions, the National Laboratories, and throughout academia. CDAC formally began operations on May 1, 2003 with the first funding year ending January 31, 2004. This report covers activities from the CDAC Academic Partners, Laboratory Partners, and University Collaborators since July 2005. Research carried out by National Lab partners, but done outside of the CDAC facilities, is not included. 1.2 Highlights from Year 3 Outreach and Training CDAC continues to make excellent progress in outreach and training, an important part of its mission. The following are highlights, in particular as it relates to students: • Facilitated continual growth of users at HPCAT. To date, more than 281 users have conducted experimental work at the sector. • Increased the number of CDAC collaborations/facility users. Some 411 outside collaborators from over 145 institutions have worked with us on Stewardship Science-related projects. • Science supported Ph.D. thesis work of 19 students at CDAC partner universities and Carnegie and encouraged career development. • CDAC student, Wendy Mao began an Oppenheimer fellowship at LANL and Jung-fu Lin began a Lawrence Fellowship at LLNL. • CDAC supported the Synergy of 21st Century High-Pressure Science and Technology Workshop at Argonne in May 2006, which featured 59 lectures from leading high pressure scientists from academia and the National Laboratories. • Hosted numerous visitors to other CDAC facilities (e.g., Carnegie and NSLS) for training and technique development and established enhanced and expanded collaborations with high pressure programs at all NNSA Labs. • Hosted undergraduate and high school interns at Carnegie and HPCAT. This past year, eight students were working on CDAC-related research projects. 4 Figure 2. Participants listen to a lecture at the 2006 Synergy of 21st Century High- Pressure Science and Technology Workshop held at the Advanced Photon Source. Scientific Breakthroughs Some 362 papers have been published since the start of the Center as a result of the support from the grant. This list includes papers describing work carried out by the CDAC Academic Partners, Carnegie research supported by the grant, and research carried out at HPCAT and CDAC facilities at NSLS. (The list does not include the large amount of research performed by high- pressure groups within the National Labs not done at CDAC-supported facilities). These papers included articles published in the major high-impact journals. • High pressure inelastic scattering of H2O reveals bonding changes and dissociation: LLNL scientists carried out direct measurements of the electronic structure of water. Complementary measurements carried out by LANL and Carnegie reveal x-ray induced dissociation2. • New findings in heavy rare earth metals at high pressure: The Alabama-Birmingham
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