100 Tesla multishot. 60 Tesla long pulse. Los Alamos branch of the Magnet Lab Pulsed magnetic fields

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1 Los Alamos branch of the Magnet Lab Pulsed magnetic fields 100 Tesla multishot Magnetic field (T) time (s) 60 Tesla long pulse time (s) Magnetization, Electric polarization, Resistivity, de Haas-van Alphen, Torque, Tunnel-diode oscillators Optical absorption & transmission etc

2 Pulsed Field Facility

3 Magnet Lab Pulsed-Field facility: ~35 people 1/3 scientists, 1/3 engineers & technicians, 1/3 students & post-docs

4 Frustration and Functionality Vivien Zapf Magnet Lab, Pulsed Field Facility Los Alamos National Lab

5 Order by disorder (Fluctuations) Static order Spin glass Spin liquid static order Static quasi-order Lattice distortions lifting the frustration Static order Order by impurity Static order Partial frustration/ Competing interactions Static order Static order near frustration: tends to complex spin textures Noncolinear Non-coplanar Long-wavelength modulations Spirals Spatially segregated phases

6 Frustrated spin systems : Complex spin textures -> broken symmetries 1. Chirality. Couple to electron transport (Hall effects) e.g. Skyrmions or other spin textures with berry phases CONDUCTORS, SEMICONDUCTORS Solid angle Ω e 2. Broken mirror symmetry: (chirality is a subset) Couple to Ferroelectricity INSULATORS 3..

7 Multiferroics Record-sensitive magnetic sensors at low powers Tunable filters, antennas, gyrators, etc. Tunable microwave devices Energy harvesting D. Khomskii, Physics 2, 20 (2009) Low power consumption Voltages instead of currents Memory/smart devices Electric manipulation of magnetic domain walls, topological objects, etc.

8 This talk 1. Nearly frustrated static order Complexity, Broken symmetries Coupling to ferroelectricity: 4 examples Microscopic mechanisms B J e J P J 4. High magnetic fields and explosions

9 Frustrated spin systems : Electric fields break mirror symmetry (SIS) A unique polar axis Is there any choice of origin for which x -> -x conserves symmetry? No: breaks spatial inversion symmetry x = 0 mirror x - + x + - x -x

10 Frustrated spin systems : Can I create a magnetic pattern that matches that of an electric field? If so, I have a chance to create ferroelectricity Cut the arrows Sorted the arrows

11 Frustrated spin systems : Exercise: Perform mirror inversion about x on this spiral Cycloidal spiral?? -x x x -x?? SIS = spatial inversion symmetry x = 0 -x - + x + - x -x

12 Exercise: Perform mirror about x on this spiral Cycloidal spiral Frustrated spin systems :? SIS = spatial inversion symmetry x = 0 -x - + x + - x -x -x x x -x

13 Spins are not arrows Spin transforms as a rotation Frustrated spin systems :

14 Cycloidal spiral Frustrated spin systems : Exercise (complete): Perform mirror inversion about x on this spiral P -P -x x x -x Breaks spatial inversion about x In the attempt to regain my original pattern, I m allowed to translate the spiral because an electric FIELD (as opposed to a dipole) conserves translational symmetry.

15 Frustrated spin systems : Some spirals that break mirror symmetry CAN BE SPONTANEOUSLY GENERATED BY FRUSTRATION (spins are in the plane of the board) Helical (with caveats) T. Kimura, Annu. Rev. Mater. Res. 37, 387 (2007)

16 Frustrated spin systems : Magnetoelectric materials with spirals T. Kimura, Annu. Rev. Mater. Res. 37, 387 (2007)

17 Frustrated spin systems : GOAL: Couple magnetism to ferroelectricity We can give magnetism a symmetry that matches an electric field But to create ferroelectricity we need to add charges to the spins Spins <-> orbits <-> lattice.

18 Frustrated spin systems : Microscopic mechanisms (usually both happen in a given material) 1. Magnetostriction [Always happens]. Let magnetic forces move charged ions around to create electric dipoles Polar bonds. Magnetic exchange bonds can have polar distribution of electron density. Frustration required + J e J H + J P +

19 Frustrated spin systems : Example 1: Dzyaloshinskii-Moryia interaction H = D z (S 1 x S 2 ) O P = 0 SIS is conserved Consequence: Cycloidal spiral Exchange tensor + H = S 1 T S 2 P O r 1 r 2 D z ~ r 1 x r 2 Broken SIS, vertically In both the spins and the bond. D z

20 Frustrated spin systems : + P O - + Mirror symmetry is broken Spins, charges separately + O P

21 Reverse cause and effect. 1. Frustration creates a spiral Frustrated spin systems : 2. Bonds distort to match magnetic symmetry (Electric polarization created as a byproduct.) + + P O Generate a DM interaction Lowers magnetic energy H = D z (S 1 x S 2 ) e ij P ~ (S i x S i+1 ) x e ij

22 Frustrated spin systems : Breaks mirror symmetry -- but not along a unique axis

23 Frustrated spin systems : Unique polar axis selected by magnetic field

24 Frustrated spin systems : Example 2: Trimers. L. N. Bulaevskii, C. D. Batista, M. V. Mostovoy, and D. I. Khomskii, PRB 78, (2008). Magnetostriction B = 0, P = 0 J J P J J B + - J J + Orbital magnetoelectric coupling. B = 0, P = 0 + J J e + J + Conserves SIS Electron of the superexchange interaction P J e J J Breaks SIS B

25 A metal-organic material with Cr trimers

26 Electron spin resonance experiments T = 4.0K Electric dipole active features associated with magnetic level crossings P J e P J B ESR The only problem with this material Is that triangles point in both direction J

27 Frustrated spin systems : D. Khomskii P=0 3-in-1-out (monopole) P P ~ δn = 8t 3 /U 3 (S 1 S 2 + S 1 S 3 2 S 2 S 3 )

28 Electric field stabilizes monopoles T (K) 3-in-1-out (monopole)

29 Frustrated spin systems : Example 2: Linear exchange striction Ni 2+ S = 1 Superexchange H = JS 1 S 2 AFM J Cl - d, J J ~ ( d) 4 to ( d) 10 for small d Maybe be linear, or due to changing the angle. If the spins are not satisfying J distort the lattice, make J smaller. Or if the spins are satisfying J, distort the lattice to make J bigger. Ni 2+ S = 1 Balance magnetic energy gain against at energy cost of lattice distortion

30 Frustrated spin systems : FM = ferromagnetic AFM = antiferromagnetic FM J AFM J FM J FM J Exercise: Place the spins so as to satisfy the bonds Assume Ising spins.

31 Frustrated spin systems : FM = ferromagnetic AFM = antiferromagnetic FM J AFM J FM J FM J Answer: It s frustrated

32 Frustrated spin systems : The lattice comes to the rescue: Frustration-lifting distortion (Similar to Spin Peierls) FM H = JS 1 S 2 J ~ d 4 to d 10 AFM J Minimize energy of spins + lattice. FM J Disclaimer: Actual distortions 1 part in

33 Frustrated spin systems : Exercise: Does it break mirror symmetry? (apply mirror vertically) x 1. Physically interchange the spins along x 2. Apply mirror inversion to the spins 3. You are allowed to vertically translate in an attempt to see if the inverted system match the original -x E Translational symmetry

34 Frustrated spin systems : mirror inversion mirror inversion + translation E x Translational symmetry CANNOT produce an electric polarization -x

35 Frustrated spin systems : Try two different kinds of spins Co 2+ y Mn 4+ y Breaks SIS Electric dipole Mn 4+ Co 2+ P Co 2+ Mn 4+ P Mn 4+ -y Co 2+

36 Frustrated spin systems : Domain 1 Domain 2 Mn 4+ Co 2+ y FM Mn 4+ y P P Co 2+ FM Mn 4+ Mn 4+ Co 2+ Co 2+

37 Ca 3 CoMnO 6 OR Two ways to distort: Two ferroelectric domains Onset of magnetic order Elastic neutron 1.4 K Y. Choi et al., PRL 100, (2008)

38 Ferroelectricity Lattice Magnetization Ca 3 CoMnO 6 Evolve, kill, and ultimately understand the magnetoelectric coupling J. W. Kim et al, PRB 89, R (2014)

39 ANNNI model (Anisotropic next nearest neighbor interactions) Ising spins have few options for satisfying competing interactions -> resort to long wavelengths Y. Kamiya & C. D. Batista very long wave lengths (~1000 A) (Each node carries an Electric polarization) Each line is a phase boundary Different (sliding) wave lengths

40 Pulsed-field measurements of the electric polarization H - - P ) I + + A ( dp / dt dh / dt Field db/dt (T/s) Time (ms) P(H) up to 65 T (95 T?) Signal to noise increases with speed of pulse Sub pc/cm 2 resolution

41 Selection of frustration-induced ferroelectrics at the NHMFL Ca 3 CoMnO 6 CdV 2 O 4 CuCrO 2 Ca 3 Co 2 O 6 and Ca 3 CoMnO 6

42 Summary Competing interactions are a source of low symmetry spin states Match the symmetry of an electric field Create multiferroic behavior P B J e J P J

43 Multiferroics Record-sensitive magnetic sensors at low powers Tunable filters, antennas, gyrators, etc. Tunable microwave devices Energy harvesting D. Khomskii, Physics 2, 20 (2009) Low power consumption Voltages instead of currents Memory/smart devices Electric manipulation of magnetic domain walls, topological objects, etc. Caveat: frustration reduces ordering temperatures, so applications mostly focus on type 1 unfrustrated multiferroics. E.g. magnetism modifies a ferroelectricity that is already present. Or: heterostructures.

44 45 Tesla DC 45 Tesla Hybrid magnet (DC), Tallahassee

45 Record Pulsed Field (non-destructive) 1.4 GigaWatts power generator: this could power Los Angeles ~ 15% 100 Tesla Power is high But energy is low 20x a few milliseconds time (s)

46 Limitation on high magnetic fields: Strength of materials 1x Released in 1 millisecond 10s of kamps, 10s of kvolts Force on a solenoid Worlds strongest steel

47 200T (microseconds): forget about saving the magnet Sample is unharmed (usually) Microsecond pulse Before After

48 800 Tesla 800 Tesla: H c2 of YBCO

49 100 Tesla The greater accomplishment: A 100 Tesla magnet that does not explode Maximize useful measurements Milliseconds

50 What can you measure in a few milliseconds? Frustrated Ca 3 CoMnO 6 Ferroelectricity Sample Length Magnetization Magnetization x less sensitive than in DC magnets Sample Length (magnetostriction) Comparable to DC measurements 1 part in 10 6 to 10 7 magnetostriction Ferroelectricity 10-1,000x MORE sensitive than DC magnets

51 Acknowledgements S. Chikara J. Singleton N. Harrison J. W. Kim C. D. Batista Shizeng Lin Giawei Chern Eun-Deok Mun Y. Kamiya J. W. Kim E. D. Mun S.W. Cheong

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