introduction to neutron spectroscopy - gdr...
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Introduction to neutron spectroscopy
Yvan SidisYvan Sidis
Laboratoire Léon BrillouinLaboratoire Léon BrillouinCEA-CNRS, Saclay
Ecole d'été MICO – AUSSOIS , 5-11 juin 2010
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Neutron scattering cross-section
Theory
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Partial differential cross-section
Definition:
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Partial differential cross-section
Neutron: no charge spin ½ plane wave energy stateno charge spin ½ plane wave energy state
Target: energy state
Scattering: initial state final state g
Kinematic constraints
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Partial differential cross-section
Probability for the incidentneutron to be in the
Density of accessible states k'
spin state |>
Neutron fluxNeutron fluxProbability for the targetto be in the initial state |>
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Partial differential cross-section
Scattering potential
Partial differential scattering cross-section
Scattering potential
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Nuclear neutron scatteringNuclear neutron scattering
ThTheory
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Nuclear scattering: scattering by a single nucleus
b= scattering lengthScattering strength
•positive or negative•depend on the isotope
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Nuclear scattering: scattering by a single nucleus
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Nuclear scattering: scattering by a single nucleus
Non magnetic scattering :
Evaluation of the term :Evaluation of the term :
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Nuclear scattering: scattering by a single nucleus
Properties of the -function:
Time dependent operator:p p
Projector:
Thermodynamic average:
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Nuclear scattering: crystal
l
lr
dR
O
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Nuclear scattering: crystal
Scattering potential :g p
i di t fperiodic arrangment of the lattice
???Organisation of atoms within the unit cell
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Nuclear scattering: crystal
Elastic term Inelastic terms
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Nuclear scattering: crystal
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Nuclear scattering: Elastic scattering cross-section
Elastic structure factorElastic structure factorcrystal structure
Debye-Waller factor
Bragg reflections in reciprocal spacegg p p
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Nuclear scattering: Inelastic scattering cross-section
D i l fDynamical structure factorphonons
creation anihilationpolarization
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Lattice vibration(1)
Atoms oscillating in harmonic potentials
Sum of all forces on a given atom
Equation of motion
SFN 2010
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Lattice dynamics (2)Mono‐atomic chain
Fourier transform Zone boundaries
Dispersion relation
Zone centers
SFN 2010
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Lattice dynamics (3)Di‐atomic chain
Fourier transform: 2 sets of equations
Optical phononOut‐of‐phase vibration
Acoustic phononIn‐phase vibrations
SFN 2010
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Lattice dynamics (3)General case
Normal coordinates
Fourier transform:
Dynamical matrix of dimension
Eigenmodes = phonons = collective vibration modes
Longitundinal modes Transverse modes
o square root of the phonon frequencyphonon frequencyo phonon polarization
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Magnetic neutron scatteringMagnetic neutron scattering
ThTheory
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Magnetic scattering potentials
Scattering potential:
Neutron: magnetic moment operator Target: distribution ofinternal magnetic fields
(1) Spins of unpaired electron(2) Electronic orbital moments(3) Nuclear spins
spin only scattering: Di l i t ti ith l t i ispin-only scattering: Dipolar interaction with electronic spins
unpolarized neutron beam:
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Partial differential cross-section
prefactor Owing to the dipolarInteraction one can observe onlyInteraction one can observe only the spin components perp. to Q
Magnetic form factor =Fourier transform of the spinpDistribution on each atom
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Magnetic structure factor
For a single type of magnetic atom
Magnetic structure factor = Fourier transform in space and time of spin-spin correlation function
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Fluctuation-dissipation theorem & detailed balance factor
Detailed balance factor
Imaginary part of the dynamical magnetic susceptibility
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Ordered magnetic moment & spin waves
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Spin wave – Magnons (1)
Ferromagnetic chain:
Hamiltonian:
Spin fluctuations:Spin fluctuations:
E f tiEqn of motion:
M fi ldMean field approx.
Eqn of motion:
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Spin wave – Magnons (2)
Fourier components:
2coupled eqns
Fourier components:Fourier components:
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Spin wave – Magnons (3)
Spin wave:
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Neutron scattering techniqueNeutron scattering technique
Th R litTheory versus Reality
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Neutron sources
-(1) a Fission reactor: a thermalneutron is absorbed by a 235Unucleus which splits into fission
-(2) spallation: A high energy proton(~1GeV) chops pieces of a heavynucleus. Twenty to forty neutronsnucleus, which splits into fission
fragments and evaporates a fewneutrons with energy of 1 to 2MeV
y yare evaporated with energies oftypically a few MeV
MeV.
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Neutron energy and wave length
Neutrons then slow down by loosing energy through inelastic collisions with light atoms (H,D,Be).
Characteristic energy (meV).0.1 - 10 meV : cold neutrons (moderator: liquid H2 at 20 K)210 - 100 meV : thermal neutrons
100 - 500 meV : hot neutrons (moderator: graphite at 2000 K)> 500 meV : epithermal neutronsV p
A neutron of 25 meV wave length of ~1.48 ºA.the same order of magnitude as the typical inter-atomic distance in a solidthe same order of magnitude as the typical inter-atomic distance in a solid.
Neutron energy same order of magnitudeas the characteristic excitations in a solid such as the phonons or the magnons.
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Neutron energy and wave length
Neutron spectroscopy can be used to probe the nuclear and magnetic structures of a sample and the related nuclear and magnetic excitations. This is a bulk and non destructive measurement.
Neutron scatering vsNeutron scatering vs. Other inelastic probes
Neutron
SR, MossBauer spectroscopy
NMR
Local probes
Magnetic excitations
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Monochromatic neutron beam
Monochromator:Monochromator:
Bragg scattering on ai l lsingle crysral
Chopper :
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Diffraction measurements : integration on the final energy
single crystals4-circle diffractometers
Powder samplePowder diffractometer
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Inelastic Measurements: analysis of the final neutron energy
Single crystalTriple-axis spectrometer
Powder samplesTime of flight spectrometerp p
(TAS)g p(TOF)
The final energy is given: ½ Mv2
v = D/.D is the fixed distance between the sample and the detector (the flight path) and the time of flight of the neutron.and the time of flight of the neutron.
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Instrumental resolution
Measured intensity proportional to
The Fourier transform of the theoretical structure factorconvoluted by the instrumental resolution function
Gaussian function (4 dimensions)Resolution ellipsoidResolution ellipsoid
Simplified description (Cooper, Nathans,1967…)Th l ti f ti d R ( XtAX)The resolution function reads : R0exp(-XtAX)X stands for a 4D vector : (Q-Q0,w-w0)
2fi01)Adet(VVR with Vi=pmki
3cot(m) et Vf=pakf3cot(a)
Vi provides the same information as the monitor fixed kf
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Instrumental resolution
Focusing effect on two modes at q and +qNeutron scattering techniqueFocusing effect on two modes at –q and +qNeutron scattering technique
f iA li tidefocusing focusing
focusing
defocusing
Applicationdefocusing
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Sr2RuO4
Superconductivity
R
La2-xBaxCuO4 Sr2RuO4
Superconductivity TC 1.5K (1994)
A i t i 3 di t lRu
OCuO
Anisotropic 3-dim. metal RC/Rab 450ab<1cm
Pauli-ParamagnetismLa/Ba Sr
12 72 Å
Fermi liquid (low T)12.72 Å
Odd parity (p-wave)Spin-triplet pairing3.86Å
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Sr2RuO4 – electronic structure
eFree IonFermi surface: 3 sheets
4d4eg
t2
Ru4+: 4d4
dyz,dxz band
t2g
Crystal Field
dxy band
Crystal Field
(2 dim.) (1 dim.)
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Sr2RuO4 – dynamical nesting
The non interaction spin or charge susceptibility is given by the Lindhardt function
jik iqjqk
jqkikji
qkkB i
ffMgq
,, ,),(
),(,,
)(;20 0
)]()([),(
,,, ji1/0Mj iqjqk,, ,),(
Strong nesting effect between the quasi-1d and bands
Qi=(0.3 0.3)
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Instrumental resolution
Focusing effect on two modes at q and +qunpolarized INS measurementsFocusing effect on two modes at –q and +qunpolarized INS measurements(single crystals)
f idefocusing focusing
focusing
defocusingLattice dynamicsdefocusing Lattice dynamics
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Sr2RuO4 – lattice dynamics
scattered intensity :
Calc lated and meas redCalculated and measureddispersion curves
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Sr2RuO4 – lattice dynamics
Lattice instability:
3 branch, which ends at the zone boundary (0 5 0 5 0) in the modeboundary (0.5,0.5,0) in the mode corresponding to the RuO6 octahedron rotation around c axis, exhibits a sharp d t th b ddrop at the zone boundary.
Sr2RuO4 is close to rotational instability
Kohn anomaly: No phonon anomaly detected at the planar nesting wave vector Q =(0 3 0 3)nesting wave vector Qi=(0.3,0.3)
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Instrumental resolution
Focusing effect on two modes at q and +qunpolarized INS measurementsFocusing effect on two modes at –q and +qunpolarized INS measurements(single crystals)
f idefocusing focusing
focusing
defocusingdefocusing
Spin dynamics
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Sr2RuO4 –spin dynamics
Magnetic scattering:
Magnetic response close to the planar nesting wave vectorplanar nesting wave vector Qi=(0.3,0.3)
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Sr2RuO4 –spin dynamics
INS
RPA
2D spin fluctuations
RPA
2D spin fluctuations
Intensity along c controlled by F(Q)2 only
INS measurements in agreement with RPA calculations
by F(Q)2 only
Intensity decreases at large |Q||Q|
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Sr2RuO4 – near a SDW instability
close to magnetic instability
1-I(qi)0(qi)= 0
0(qi)
t l Tat low T
Sidi t l PRL 83 3320 (1999)Sidis et al. PRL 83, 3320 (1999)Braden et al. PRB 66, 064522 (2002)
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Sr2RuO4 – origin of non Fermi liquid
T* TN
p-wave SC
Fermi Liquid SDW
p wave SCQCP
T>T* /T liT>T* /T scaling
Non Fermi liquid : T>T* , ~Tq ,
Fermi liquid : T<T* , ~T2
Braden et al. PRB 66,064522 (2002)
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Instrumental resolution
Focusing effect on two modes at q and +qPolarized INS measurementsFocusing effect on two modes at –q and +qPolarized INS measurements(single crystals)
f idefocusing focusing
focusing
defocusingdefocusing
Spin dynamics
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Sr2RuO4 – polarized INS measurements
Spin polarized neutron beam
H
Heusler monochromator / analyzer
Single domain ferromagnet
|b | |b ||bN | = |bm|
Interference between nuclear and magnetic scattering
| b + b |2 0| bN + bm|2 = 0
| bN - bm|2 ≠ 0
A magnetic guide field keep the spin polarization and defines the polarization P of neutron spin
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Sr2RuO4 – polarized INS measurements
Polarization:
Nuclear scattering : non spin flip scattering
Magnetic scattering: spin components: (i) Q , (ii) P spin flip scattering
(0 0 1) S i fli h l
HHz
( ) Spin flip channel :
Ix ~ Im a,b + Im c + Bg
I ~ Im + Bg
Hx
Hy
(0 1 0)
Iy ~ Im c + Bg
Iz ~ Im a,b + Bg
Q
H P // Q
(100)
Hx : P // Q
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Sr2RuO4 – spin anisotropy
(0 0 1)
Polarized neutron 8 meV
Hy
Hz
QHx
(0 1 0)
Q
Hx : P // Q
(1 0 0)
x
Anisotropy of IC spin fluctuations at Qi
c(qi) / a b(qi) ~1.6spin orbit coupling c(qi) a,b(qi)spin-orbit coupling
+ strong correlation
c(qi) / a b(qi) >1anisotropic spin fluctuations can favor spin tripet SC
Ng et al. J. Phys. Soc. Jpn, (2002).Manke et al., PRB (2002).
c(qi) / a,b(qi) 1 p p
Sato et al. J. Phys. Soc. Jpn, (2000).Kawabara et al., PRB (2000).
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Sr2RuO4 – full spin susceptibility
’(q,0)60
80
100
T = 150 KE = 8 meV
eV-1)
60
80
100
T = 1.6 KE = 8 meV
eV-1)
0
20
40
'' ( B
2 e
0
20
40
'' ( B
2 e
80
100
T = 150 KE = 15 meV
0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.30
(Qh, Qh-1, 0)
80
100
T = 1.6 KE = 15 meV
0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.30
(Qh, Qh-1, 0)
20
40
60
'' ( B
2 eV
-1)
20
40
60
'' ( B
2 eV
-1)
0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.30
20
(Qh, Qh-1, 0)0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 1.30
20
(Qh, Qh-1, 0)
Broad and weak excitationsaround Q=0 (~20 meV)
band
sharp and strong excitations
Hx : P // Q – spin flip channel
around Qi (~7 meV)
bands
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Instrumental resolution
Focusing effect on two modes at q and +q
INS measurementsFocusing effect on two modes at –q and +q
f i
Versus
defocusing focusing
focusing
defocusingNMR
S ifi h defocusing Specific heatARPES
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Sr2RuO4 – NMR – local probe
S i l tti l ti
INS
Spin-lattice relaxation
Hyperfine coupling
NMR NMR
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Sr2RuO4 – specific heat
Spin fluctuation contributionAt low temperatureAt low temperature
IC
FM
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Sr2RuO4 – charge excitations - ARPES
ARPES : spectral function of quasiparticles
Scattering : self-energy
collision with bosonic modes (phonons spin excitations )(phonons, spin excitations,....)
: characteristic energy of bosonicManske et al., PRB 67, 134520 (2003)Manske et al., PRB 65, 220502 (2002)
: characteristic energy of bosonic modes ( phonons or spin excitations)
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Sr2RuO4 – charge excitations - ARPES
Iwasawa et al., condmat/0508312
ARPES
observed Kink in the bandsf~25meV
Role of the pseudo-FM fluctuations ?...... Role of phonons?
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Instrumental resolution
Focusing effect on two modes at q and +q
Unpolarized elastic measurements(single crystal)Focusing effect on two modes at –q and +q(single crystal)
f iMagnetic orderdefocusing focusing
focusing
defocusing
Magnetic orderdefocusing
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Sr2RuO4 – order from disorder
QCP
N ti Ti 4+
Magnetic wave vector q0Non magnetic Ti 4+ vector q0
Intensity proportional Orientation factor gives the direction of Correlation length y p p
to the square of the order moment
gives the direction of the order moment
gq ~-1
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Sr2RuO4 – order from disorder
Study : Q= qo+ q =(0.307,0.307,1) , = (1 0 -1) [I4mmm structure]
Ordered moment: m = 0.3 B Néel temperature : TN = 25 K
Planar correlation length : a b ~50 ÅPlanar correlation length : a,b 50 Å
along c : hardly correlated system
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Sr2RuO4 – mag. Order vs Fermi surface
q =(0.307,0.307, 1)
The order wave vector is 3D
Modulation along c of the and (i l d i ti ) (involved in nesting)
C. Bergemann et al.
dHvA
C. Bergemann et al.
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Sr2RuO4 – spin density wave
M1 : SDW with m // c
M4 : helimagnetFULLPROF- program
magnetic Moments are // to cconsistent with the spin anisotropy observed in Sr2RuO4consistent with the spin anisotropy observed in Sr2RuO4
Origin: spin-orbit coupling
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Instrumental resolution
Focusing effect on two modes at q and +q
Powder diffraction measurementsFocusing effect on two modes at –q and +q
f iMagnetic and nuclear structures
defocusing focusing
focusing
defocusingPh di defocusing Phase diagram
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Ca2-xSrxRuO4: Structural properties
r = 1.31ÅSr2+r = 1.18ÅCa2+Isovalent substitution rCa < rSr
rotation and tiltrotation
rotation and tilt
Sr RuOCa RuO Sr2RuO4Ca2RuO4
Nakatsuji et al. PRL 84 2666 (2000), Friedt et al. PRB 63, 174432 (2001), Braden et al. PRB 58, 847 (1998)
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Ca2RuO4: Nuclear structure
Incident neutron beam
2
Bragg reflections : Ca2RuO4
Bragg reflections: CaRuO3 (impurities)
Friedt et al. PRB 63, 74432 (2001),Braden et al. PRB 58, 847 (1998)
(impurities)
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Ca2RuO4: Magnetic structure
Mott Insulator Ca2RuO4 : T<Tn, A-type AF order
Magnetic moments // b = elongation of octahedrag g
Magnetic moment ~1.3 B < 2B (localized S=1 , Ru4+)
Friedt et al. PRB 63, 74432 (2001),Braden et al. PRB 58, 847 (1998)
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Instrumental resolution
Focusing effect on two modes at q and +q
Polarized neutron diffraction (high quality sample)Focusing effect on two modes at –q and +q(high quality sample)
f iSpin density mapsdefocusing focusing
focusing
defocusing
Spin density mapsdefocusing
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Ca2-xSrxRuO4: meta-magnetism
Intermediate Sr Content
0.2 < x < 0.5
i i bili
Metallic state
• near magnetic instability• high specific heat•metamagnetic transition
• octahedra tilt
Band structure : narrowing of the bandvan Hove singlarity shifts below Efvan Hove singlarity shifts below Ef
Hall measurementsSign change of charge carriersSign change of charge carriers
Nakatsuji et al. PRL 90 (2003)
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Ca2-xSrxRuO4: spin density map
I+
D
M F H
I-
2I+ N MF +FR
I± ( FN ±FM ) 2
FM << FN
I- N MF -FR
R 1 4 MF FM << FNNF
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Ca2-xSrxRuO4: spin density map at x=0.5
0.35 B Ruthenium 4dxy orbitals ( band) 0.08 B Oxygen (in-plane) significant amount of magnetization on oxygen0.01 B Oxygen (apical)
RuO2 plane:
0.01 B Oxygen (apical)
4
2
-2
0
-4O
-4 -2 0 2 4Å
Ru
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Instrumental resolution
Focusing effect on two modes at q and +q
Inelastic neutron scattering(single crystal)Focusing effect on two modes at –q and +q(single crystal)
f iExternal magnetic fielddefocusing focusing
focusing
defocusing
External magnetic fielddefocusing
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Ca1.8Sr0.2RuO4: meta-magnetism
INS: Ca1.8Sr0.2RuO4
Sr2RuO4
Steffens et al. Cond-mad(2010)
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Ca1.8Sr0.2RuO4: meta-magnetism
180
210
8 meV
150
180
6 meV
90
120
150
6 meV
unts
90
120
150
ts
4 meV
30
60
90
4 meV
co
30
60
90
count
2.5 meV
-0.6 -0.4 -0.2 0.0 0.2 0.4 0.6
0
2 meV
Q = (1, K, 0) 0.6 0.8 1.0 1.2
0
Q = (H, H-1, 0)
(1 0 0)
Steffens et al. Cond-mad(2010)contributions from several Q(q1=0.12, q2=0.27)
Q (H, H 1, 0)
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Ca1.8Sr0.2RuO4: meta-magnetism
120 B || bT=2K8T Fundamental change of magnetic fluctuations at
80
100
6T
metamagnetic transitionIC FM
60
80
ts
6T
FM
IC
40
count
3T-0.5 0 0.5
H
AFMIC
20
0T
-0.4 -0.2 0.0 0.2 0.4
0
Q (H 0 1 6) E 2 V
Steffens et al. Cond-mad(2010)
Q = (H, 0, 1.6) E=2meV
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Ca1.8Sr0.2RuO4: FM-magnons
210B = 10 T
B c T=2K
4 meV18 0
21 0
B c T= 2K
2 m eV
150
180
3 meV5
)
12 0
15 0
nts
B = 1 0 T
120
150
ts
2
3
4
E
(meV
)
3 0
6 0
9 0
B = 0
coun
B = 6 T
60
90count
2.5 meV-0.1 0.0 0.1
1
K-0 .6 -0 .4 -0 .2 0 .0 0 .2 0 .4 0 .6
0
0
Q = (1 , K , 0 )
30
60
2 meVDispersive mode (Magnon) = D q2
-0.6 -0.4 -0.2 0.0 0.2 0.4 0.6
0
Q = (1,K,0)
q
Field induced FM state
Steffens et al. Cond-mad(2010)
Q ( , , )
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Ca1.8Sr0.2RuO4: structural effects
Distortion of the octahedron
cooling
e-
field
e-
field
xy xz,yz
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+0 06eVMagnetismof -band
+0.05eV
+0.06eV
+0 07eV
+0.025eV
+0.07eV
0 eV
+0.085eV
+0.1eV0 05 V-0.05eV
-0.1eV
+0.15eV
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Instrumental resolution
Focusing effect on two modes at q and +qFocusing effect on two modes at –q and +q
f idefocusing focusing
focusing
defocusingdefocusing