Infrastructure for QIS Research DOE’s Light Sources, Neutron Sources, and Nanoscale Science Research Centers National Quantum Initiative Community Meeting | December 8, 2020

STEPHEN STREIFFER Deputy Laboratory Director for Science & Technology Interim Associate Laboratory Director, Photon Sciences Director, Advanced Photon Source Argonne National Laboratory at a Glance FY 2020 Enacted: $7.0B + $99.5M (CARES Act)

Largest Supporter of Funding at >300 Institutions, Over 23,000 Researchers Over 36,000 Users of Physical Sciences in the U.S. including 17 DOE Labs Supported 28 SC Scientific Facilities

~38% of Research to Research: Facility Operations: Projects/Other: Universities 38.8%, $2.7B 36.4%, $2.5B 24.9%, $1.7B

2 2 Office of Science User Facilities • A SC user facility is a federally sponsored research facility available for external use to advance scientific or technical knowledge under the following conditions: – The facility is open to all interested potential users without regard to nationality or institutional affiliation. – Allocation of facility resources is determined by merit review of the proposed work. – User fees are not charged for non-proprietary work if the user intends to publish the research results in the open literature. Full cost recovery is required for proprietary work. – The facility provides resources sufficient for users to conduct work safely and efficiently. – The facility supports a formal user organization to represent the users and facilitate sharing of information, forming collaborations, and organizing research efforts among users. – The facility capability does not compete with an available private sector capability. https://www.energy.gov/science/science-innovation/office-science-user-facilities https://science.osti.gov/User-Facilities https://science.osti.gov/User-Facilities/User-Facilities-at-a-Glance/BES

3 3 FY 2021 28 Scientific User Facilities 36,000+ users OLCF ALCF NERSC ESnet

EMSL ARM JGI SNS HFIR

ALS APS LCLS NSLS-II SSRL

CFN CINT CNM CNMS TMF

DIII-D NSTX-U FACET ATF AC

CEBAF ATLAS RHIC FRIB 4 4 Basic Energy Sciences Light and Neutron Sources

Spectroscopy of for Nanoscale structure Electronic Structure, Magnetic structure composition and and strain excitations chemical state

National Light Source II Linac Coherent Light Source Stanford Synchrotron Radiation Light Source Brookhaven National Laboratory SLAC SLAC

Spallation Neutron Source High Flux Isotope Reactor Advance Light Source, Advanced Photon Source Oak Ridge National Laboratory Oak Ridge National Laboratory Lawrence Berkeley National Laboratory Argonne National Laboratory

5 BES Nanoscale Science Research Centers

Electron Optical microscopy Scanning Materials Nanofabrication spectroscopy for materials probes synthesis characterization

Center for Integrated Nano Technologies The Molecular Foundry Sandia, Los Alamos Lawrence Berkeley Laboratory

Center for Functional Nanomaterials Center for Nanophase Center for Nanoscale Materials Brookhaven National Laboratory Oak Ridge National Laboratory Argonne National Laboratory

6 Accessing BES User Facilities § Prospective user submits a proposal to facility • Proposals are typically short – 3-5 pages – describing importance of proposed work, estimate of time required to complete work, requested /instrument • Life of the proposal typically 1-2 years (depending on facility) or a 1-time experiment (sometimes called rapid-access proposals) • Proposal can be non-proprietary (no user fees) or proprietary (user fees applied)

§ Proposal goes through review process managed by facility • Proposals are evaluated on feasibility and merit of proposed work – criteria set by individual user facility • May be different review processes for different types of proposals (e.g., proprietary, non-proprietary proposals, rapid access, etc.)

§ Successful proposals are allocated time on requested beamline/instrument

7 Requirements Before/After the Experiment § Before start of experiment: • All users must have a completed User Agreement between their home institution and the facility – 2 types of User Agreements – proprietary and non-proprietary • A Safety Form is submitted by PI describing any hazards associated with experiment and any hazard mitigations (if necessary), and approved by facility representatives • All users associated with experiment must have completed facility’s required training

§ After completion of experiment: • Users acknowledge use of facility in any publications resulting from data obtained from access to facility • Users notify facility of those publications

8 DOE’s Light Source Network

Impact by the Numbers Product breakthroughs: • ~ 11,000 users each year HIV & cancer drugs, green refrigerants, improved • From all 50 states, ~33 countries LEDs, green energy, thin films, batteries, gasoline • Oversubscribed by factor of 3 or 4 injector system • More than 250 universities • More than 200 companies, many Fortune 500 Government partnerships: • 4 Nobel Prizes DOE, NIST, NSF, NIH, NNSA, DOD, NASA Storage Rings Soft(est) X-Rays Intermediate Wavelength Hard X-Rays X-Ray Lasers

Surface and Diverse range of Studies of real materials, Full spatial coherence, electronic structure characterization and systems, and processes in real ultrafast dynamics in exploration time under real conditions molecules and materials

ALS NSLS-II & SSRL APS LCLS

Each has unique characteristics as well as tailored overlap of certain capabilities, to cover the entire discovery space for a broad user base The Advanced Light Source at Lawrence Berkeley National Laboratory

The ALS uses photons from the infrared to the hard x-ray to investigate the coupling between structure, electronic, magnetic, and lattice properties that are fundamental characteristics of quantum coherent systems, and the interaction of materials with their environments through study of temperature and field-dependence.

Spin Crossover in T-dependent Topology in Molecular States Order Parameter van-der-Waals X-ray Spectroscopy & Scattering High Fluctuations Materials Chemical Spectroscopy Spin Magnetic Spectroscopy Orbital Order Long Range Order Dynamical Structure

Factors Low Spin

photon energy(eV) Photoelectron Spectroscopy Chemical Spectroscopy Spin/Electronic Bands Lifetime Renormalization Exotic Quantum Phases Wavefunction Mapping In operando measurements Entangled 5-Dimensional characterization of device-relevant electronic states with world-leading spatial resolution

R. Koch to be submitted 2017 The Advanced Light Source at Lawrence Berkeley National Laboratory

The ALS uses photons from the infrared to the hard x-ray to investigate the coupling between structure, electronic, magnetic, and lattice properties that are fundamental characteristics of quantum coherent systems, and the interaction of materials with their environments through study of temperature and field-dependence.

Applications of ALS Tools to materials issues at the Quantum Systems Accelerator:

Investigation of the chemical origins of performance limiting noise in superconducting q-bits, ion traps, and sensors.

Mehta et al Nature 586, 533-537 (2020)

Accelerating Basic Science & Discovery by revealing the structure-dependent properties of complex quantum matter such as novel engineered superconductors, spin-orbit-valley interactions, and protected states in topological materials. β-Bi4I4 , Nature Materials 2016 / Autès et al Geim/Nature SSRL ARPES at Beamline 5: SSRL A State-of-the-Art Facility for Studying Quantum Materials

§ Excellent control of the photon polarization § Unique combination of two complementary branch lines • PGM branch line: high flux, wide photon energy (20-200 eV), small beam spot • NIM branch line: ultrahigh res. (<2 meV), low photon energy (7-35 eV), excellent beam stability § State-of-the-art ARPES end station • Micro-ARPES capability with DA30 analyzer • 6-axis low-temperature sample manipulator (10-400 K) § Sophisticated materials synthesis chamber • In situ thin-film growth, transfer, and characterization • Oxide MBE, chalcogenide MBE, STM/STS Þ Enable rich science with both depth and diversity; open doors to future applications • High-Tc cuprates, Fe-based superconductors… ARPES • Topological materials, transition metal dichalcogenides… Oxide MBE • Novel low-dimensional materials, surfaces, and interfaces… 7-35 eV > 1×1012 ph/s @ 10,000 RP E/ΔE~20,0 32(H)×5(V) µm2 (FWHM) 00 20-200 EPU eV 11 LH, LV, CL, CR M0 > 2×10 ph/s @ 10,000 RP E/ΔE~40, 0.2(H)×0.1(V) mm2 (FWHM) M1 000 M2 Apertures STM/STS VLS Gratings Chalcogenide MBE M3 NIM branch line 5-4 PGM branch line 5-2 SSRL SSRL Resonant Soft X-ray Scattering (RSXS) at Beamline 13-3

§ Unique combination of conventional RSXS capability and a state-of- the-art detector • Superconducting transition-edge sensor (TES) detector has been integrated in the RSXS setup • Delivers a highly efficient detecting mode via single photon sensitivity § Novel approach to detect glassy (weak) order • Subtraction of fluorescence background via the 2-D area (CCD) • 4-circle diffractometer and low-temperature sample environment (10-400 K) allow precise exploration of weak signals § Cutting-edge science

• Exploring intertwining ordering in high-Tc cuprates • Exploring interface phenomena in emergent heterostructures

BL13-3 branch

• Beamline parameters - Energy range: 230 – 2400 eV - Energy resolution (E/ΔE): 8000 Elliptical Polarization Undulator - Spot size: ~ 0.02 (v) X 0.5 (h) mm2 (EPU) NSLS-II – for Quantum Information Science

• Largest medium-energy synchrotron in the world, offering state-of-the-art performance from far-IR to hard x-ray energies • World-leading spatial (10 nm) and energy (14 meV) resolutions for X-rays • Leading capabilities to study strain, defects, impurities and low-lying excitations in QIS relevant materials, including SC qubits • All capabilities and expertise to use them available in General User program • Partner with DOE Co-design Center for Quantum Advantage (C2QA)

14 NSLS-II Applications to Quantum Materials

Ex 1: Decoherence times in SC qubits Materials problems: • Defects �� • Native oxide layers = = � ∑� + �0 �� • Interfacial reactivity • Surface and interface roughness

Multimodal studies underway at NSLS-II to understand and control decoherence times “Microscopic Relaxation Channels in Materials for Superconducting Qubits”, arXiv:2004.02908 Premkumar et al. Ex 2: Electronic properties of novel quantum materials Bi2Se3

• Driven skyrmion dynamics • Low-energy collective excitations • Spatially-resolved quasi-particle dispersions Advanced Photon Source QIS research Highest energy DOE light source; APS-U will make it world’s brightest storage ring.

High Energy Brightness/Coherence Time-Resolved Studies Penetrating bulk materials Highest possible spatial Measurements from and operating systems resolution/dynamics ~100 ps to seconds

§ Understanding growth and § Ability to probe nanometer features § Probing dynamic lattice synthesis of new QIS materials around QIS-engineered defects, perturbations near optically active with structural, chemical, magnetic, defects in semiconductors § Creating novel quantum states in and electronic sensitivity extreme environments (i.e. M, P, T)

16 IMAGING ACOUSTIC WAVES IN QUANTUM MATERIALS

Acoustically driven defect photoluminescence

Pulsed nano-focused x-rays were frequency matched to a driven Measured slope of the surface wave displacements 352-MHz surface acoustic wave in 4H-SiC and scanned to obtain transverse (top) and longitudinal (bottom) to the wave a real space map of the lattice displacements propagation direction SJ Whiteley, FJ Heremans, G Wolfowicz, D D Awschalom and M. V. Holt , Nat. Comm. 10, 3386 (2019). SJ Whiteley, G. Worfowicz, C.P. Anderson, et al., Nat. Phys. 15, 490 (2019) LCLS and Quantum Information Science LCLS MeV UED Instrument LCLS Nonlinear X-ray Scattering atomic-scale distortions associated with decoherence of quantum states and EFRC for Quantum switching of topological phases Sensing & Quantum Materials (QSQM)

P. A b b amo nte

Thrust: Nonlinear X-ray probing of quantum phases M. Trigo, D. Reis SLAC

Interlayer shear displacements Weyl metal topological switch E. Sie et al., Nature 565, 61 (2019) LCLS and Quantum Information Science LCLS Quantum Materials Science Campaign Ultrafast X-ray Scattering & Spectroscopy Fluctuations, Emergence and Dynamics of Complex Topological Superstructures V. Gopalan et al. (PSU, ANL, SLAC, LBNL)

topological polar structures Extreme scale characterization of quantum states: Science Objectives: and superlattices Fundamental limits of decoherence, dissipation and noise • Map collective modes Focus Area 1: of quantum polar vorticies phase field Atomic-scale characterization, creation and control of active and Skyrmions – atomic quantum defects displacements • Driven transformation Focus Area 2: pathways to super-crystal and super-crystal Visualization of quantum transduction material processes and metastable states phase field dynamics • Roll of stochastic fluctuations in emergence and erasure of LCLS ultrafast coherent X-ray methods & instrumentation: topological quantum Picometers, picoseconds, element/chemical specificity of local structures and phases quantum state environment Skyrmions Oak Ridge National Laboratory Operates Two Neutron User Facilities http://neutrons.ornl.gov

High Flux Isotope Reactor (HFIR) Spallation Neutron Source (SNS) Intense steady-state neutron flux World’s most powerful beams of and a high-brightness cold neutron source pulsed neutrons

Neutron scattering measures the structure and dynamics of materials. It is sensitive to both light and heavy atoms and to magnetism. ORNL’s neutron facilities enable various measurements on quantum materials including: • Diffraction – atomic arrangements and magnetic structures • Small Angle scattering – mesoscopic structures • Spectroscopy – collective excitations in interacting systems

20 Typical Applications of Neutrons to Quantum Materials

• Determining types of long and short range magnetic order and the arrangements of magnetic moments

• Characterizing topological structures such as vortices or skyrmions

• Measuring magnetic excitations to determine Hamiltonians and identify potentially useful quasiparticles

The Quantum Science Center will use neutron scattering for several applications: • Characterizing magnetic Weyl semi-metals and topological superconductors • Providing data on the dynamic susceptibility of quantum magnets as to validate quantum computations • Studying quantum spin liquids that might host magnetic non-abelian anyons useable as topologically protected qubits

21 Nanoscale Science Research Centers Quantum Information Science at CINT

Implant for color centers and spins

Quantum Sensed NMR • Deterministic Placement and Discovery Platform Integration of Defects

• Quantum sensing

• Transduction Rb atom to SiV

• Materials and devices for quantum Atomic lithography systems

23 QIS Differentiating Capabilities

Theory for Correlated Systems Quantum Information Science • Techniques for strongly correlated models • Quantum Transport and qubits • Many-body approaches • Quantum Sensing • Mean-field modeling for quantum materials • Focused ion implantation

Forefront Lithography Materials synthesis • Atomic-Precision Lithography • Ultra-High Mobility MBE • Nanoscale devices • Complex Oxide PLD • CVD Growth

24 QIS Scientists have a Broad Range of Expertise

Quantum Materials Synthesis, Theory and Characterization Quantum Information Science J. Yo o ** LCVD nanowire and thin-film growth M. Lilly* Quantum transport, sensing

A. Mounce Quantum sensing, NMR, spin qubits J. Zhu Quantum materials theory

T. Lu Single e- transport in low-d systems S. Trugman Quantum materials theory Matt Eichenfield Quantum transduction J. Reno III-V molecular beam epitaxy

Nanoscale Systems and Integration A. Chen Nanocomposite synthesis T. Harris Thermal and electrical transport Wanyi Nie Perovskite materials properties E. Bielejec Ion implantation E. Bussmann Atomic manufacturing, STM J. Nogan Integration lab manager W. Pan Topological materials characterization * Science Thrust Leader ** Science Co-Thrust Leader P. S . R o s a Correlated materials and emergent phenomena 25 Quantum Information Science Capabilities at the CNM The CNM has expertise and a suite of capabilities targeting three key research areas in QIS:

Single-photon emitters for Quantum transduction Spin-based systems – readout quantum optics and control

Crosscutting: Machine learning and artificial intelligence approaches to QIS; AI integration with novel QIS hardware Quantum Information Science Capabilities at the CNM Single-Photon Microscopy Ultralow Temperature Spectroscopy • QIS Purpose: Optical domain • QIS Purpose: Microwave and readout and/or control of spin states; millimeter spectroscopy of spin photon correlation microscopy states in quantum materials • 9-T single-=axis superconducting • Dilution refrigerator with 10-mK magnet base temp and 5-1-1 T magnet • Single-photon detectors covering • Adiabatic demagnetization visible to near-infrared refrigerator (ADR) with 25-mK base temperature, 5 T single axis magnet, and fast cooling

Hard X-ray Microscopy (with CNM and APS) QIS Theory and Modeling • QIS Purpose: Correlation of strain • QIS Purpose: Discover/predict with QIS function (e.g., qubit QIS phenomena; analyze and resonance energy and coherence) interpret QIS experiments • Hundredths-of-picometer strain • Enable AI/ML approaches to QIS sensitivity in 2D and 3D using Bragg • “Carbon” is a 2,600 core + 16 diffraction and Bragg ptychography GPU HPC cluster; collaborations • AI-enabled image reconstruction with ALCF also possible

Additional QIS support capabilities: Quantum material synthesis and nanofabrication, integration of quantum materials into functional QIS structures via nanofabrication, pulsed spin resonance spectroscopy, ultrafast electron microscopy, ultrafast optical spectroscopy Frontiers in Materials for Quantum at the Molecular Foundry

Atomic-scale coherence control Materials Structure-property optimization Qubits Qubit material discovery Bottom-up functionalization for computing, detection, sensing

Quantum Sensing: enhancing resolution and signal/noise; new insights into materials properties/phenomena Quantum Noise: characterizing, measuring, disentangling Coherent Processes in Materials, Chemistry & : what are the fundamental limits to coherence and entanglement in different environments?

Single photon sources in Quantum Materials for Atomically well-defined color 2D materials Dark Matter Detection & centers in 2-D materials Weber-Bargioni, Ogletree, Quantum Sensors Weber-Bargioni, Neaton Schwartzberg Griffin DOE EFRC NPQC DOE EFRC NPQC DOE-HEP QuanTISED 1. 2D Mater. 7, 031003, 2020 1. Sci. Adv. 6: 2020, 1. PRD 101, 055004 (2020) 2. arXiv:2008.12196v1 2. Appl. Phys. Lett. 117, 2. PRD 98 115024 (2020) 2020 QUINTESSENCE: Quantum Instrument for Novel Techniques Applying Entanglement and Spin-polarization for Studies with Low Energy Coherent Electrons

Creating worldwide unique quantum-SPLEEM User Instrument: user application tools: under construction, delivery April Þ Ultra-high resolution 2021 electron spectroscopy Þ QIS with entangled electrons Þ No-invasive surface analysis Þ Decoherence studies for quantum materials

New User-Instrumentation: Electron emitter characterization setup

Allows Users to develop new (quantum) electron beam sources and test them for: Bob Ø Brightness, energy Secure quantum communication distribution, by electron matter-wave Alice electron correlation modulation and coherence Eve Nanofabrication Toolset for Correlating Coherence to Structure

Understanding interfaces Ongoing internal and user work has Deposition cluster for experimental E-beam writer for large area, high demonstrated the importance of materials and interface exploration resolution device patterning materials interfaces on superconducting • Explore in-vacuo deposition to Qubit devices preserve interfaces • Test ALD based materials and passivation • New materials for wide range of • Microwave resonators are QIS applications used to probe system loss • Coming January 2022 • High resolution microscopy • Ideal system for rapid reveals presence of Dilution refrigerator for testing prototyping and fabrication of uncontrolled oxide growth superconducting qubit devices parallelized 3-dimensional superconducting qubit • Fabrication techniques • Low temperature devices used to modify interfaces superconducting device and demonstrate • User resource for qubit exploration significantly enhanced device exploration • User accessible testing facility performance • Installation underway • Coming June 2021 CNMS Recent Science Highlights

Correlating 3D atomic defects and electronic Understanding superconductivity in confined Bottom-up synthesis of atomically precise properties of 2D TMDs atomically thin half-van der Waals metals graphene nanoribbons for entangled spin states a d

SiC

b

c

For the first time the 3D bond distortion and A new strategy to creating air-stable, wafer scale Decoupled, atomically precise graphene 2D metals (Ga) at the interface of silicon carbide nanoribbons (GNRs) are obtained by the on- local strain tensor induced by single dopants in surface synthesis approach on a model metal and epitaxial graphene for novel quantum and Re-doped MoS2 monolayers were obtained with oxide, showing spin-polarized magnetic states. pm precision information sciences.

X. Tian et al, Nature Materials 19, 867 (2020) N. Brigg et al, Nature Materials 19, 637 (2020) M. Kolmer et al, Science 369, 571 (2020)

31 CNMS/ORNL recent investments in quantum capabilities

Cathodo- Spin-polarized Velion FIB-SEM Monochromated Analog quantum luminescence scanning tunneling Advanced Litho & aberration- simulator microscope microscopy (with Direct Write System corrected (MAC)- • Ion trap based • Near-field spectral, dilution refrigerator) • 10-50nm Spatial STEM platform (40Ca+) polarization, spatial, • T down to 30 mK Resolution over 2-35 • Energy resolution: • Direct temporal, and keV <10 meV at 100 kV • Vector B field = 9, 2, implementation of angle-resolved ~4 meV at 30 kV Hamiltonian characterization 2 T • Continuous writing strategies, sub 10 nm • Spatial resolution: evolution • • Spectroscopy (300- Enables access structure veracity 0.13 nm at 30 kV; to magnetic states • Reconfigurable 1000 nm), single 0.08 nm at 100 kV connectivity enables photon detection and spin • 3D nanoscale entanglement manufacturing by frustrated spin system (400-1700 nm), cryo- simulation cooling (8-300K), sub- focused ion beam ps time-resolution induced deposition • e-beam patterning • Isotopic and and e-beam vacancy induced deposition engineering for Q- materials

32 New Opportunity: Nanoscale Materials Science Infrastructure for QIS Overarching goal: develop a rapid exploration platform for the synthesis and characterization of quantum systems with entangled states in space and time domains for QIS using: CL-SEM platform: ultrafast carrier dynamics for quantum emission at localized defects. Optical (Raman, PL, etc.) Sample and target station loading / parking

XPS, XPD SPARC: High-performance SEM CL detector

FEI Quattro S

Legacy oxide chamber with laser heating Robotic transfer hub

Vacuum suitcase for New QIS chamber with laser heating and SP-STM platform: entangled transferring samples to CL- multiple beams/targets for PLD-based spin states at sub-K with SEM or SP-STM platform codeposition atomic resolution.

AI-guided synthesis platform: PLD- incorporates in situ diagnostics, as well as composition/structure and optical as inputs for AI-based decisions. Unisoku USM 1600 33 Light and Neutron Source Upgrades

QUESTIONS?