Angle-resolved photoemission spectroscopy on emergent …spin/course/106F/Lecture 9 ARPES of... ·...
Transcript of Angle-resolved photoemission spectroscopy on emergent …spin/course/106F/Lecture 9 ARPES of... ·...
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Angle-resolved photoemission spectroscopy on emergent quantum materials
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Part -1
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Outline
• Introduction to angle-resolved photoemission spectroscopy (ARPES)• The principle of ARPES• Current status of ARPES beamline at NSRRC
•The electronic structure of emergent materials• Surface states and quantum well states• Graphene based materials• Beyond graphene : 2D materials• Topological insulators (TIs)• Toward future electronic devices
•Summary
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What is photoemission?
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The energy level of hydrogen atom
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Kyle Shen, IGERT Lecture 2008
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Xeon gas phase test
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The crystal structure and momentum space
Z. Hussain, ALS summer school
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primitive vectors a1, a2, a3
reciprocal lattice vector b1,b2,b3
321
213
132
321
2
2
2
aaaV
V
aab
V
aab
V
aab
reciprocal lattice G :
321 bnbmblG
l,m,n are any integers
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Kyle Shen, IGERT Lecture 2008
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Band theory
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RT ~ 25 meV
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Hufner, Very high resolution photoelectron spectroscopy
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Why ARPES - key technique for the electronic structure mapping
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‒ Angle-resolved photoemission spectroscopy (ARPES) is the most general tool to probe band structure, electronic interactions or spectral function mapping.
‒ Broad applications: surfaces, thin films, bulk materials, superconductors, magnetic/spin systems, complex materials, topological insulators, graphene based materials, charge density wave materials, low-dimensional systems, artificial stacks, device configurations, etc.
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γ1
γ0
γ4γ3
(b)(a)
Ԧ𝑎1Ԧ𝑎2
A1B1
B2A2
x
y
The unit cell of graphene
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H 𝑘 =
𝐸0 + ∆ 𝛾0𝑓(𝑘)
𝛾0𝑓∗(𝑘) 𝐸0
𝛾1 𝛾4𝑓∗ 𝑘
𝛾4𝑓∗(𝑘) 𝛾3𝑓(𝑘)
𝛾1 𝛾4𝑓(𝑘)
𝛾4𝑓(𝑘) 𝛾3𝑓∗(𝑘)
𝐸0 + ∆ 𝛾0𝑓∗(𝑘)
𝛾0𝑓(𝑘) 𝐸0
𝑓 𝑘 = exp Τ𝑖𝑘𝑥𝑎0 2 3 + 2exp( Τ−𝑖𝑘𝑥𝑎0 2 3)cos( Τ𝑘𝑦 2)
𝑘 = (𝑘𝑥, 𝑘𝑦)
SWMc Hamiltonian of bilayer graphene
A. Gruneis et al., PRB (2008)
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Pure 2D material : graphene
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Coletti et al., PRB (2013)
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Constant energy mapping
Coletti et al., PRB (2013)
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Fermi Surface
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Why orientation of solid so important
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How to probe the electronic structure of solids
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)cos(5123.0 0
2 VEk kin
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Conservation of linear momentum parallel to the surface
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sin5123.0
)cos(5123.0
//
0
2
kin
kin
Ek
VEk
• Low photon energy provides better momentum resolution, but the covering range of BZ is also small.
• We expect to study the electronic structure of solids at VUV region (10 eV~ 100 eV).
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Krempasky et al., JESRP (2010)
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Assume the work function is 4.3 eV , please estimate the largest covering range of BZ at the Fermi level at 6 eV, 21.2 eV, 50 eV, 100 eV and 500 eV photon energy.Answer: 0.67 Å -1, 2.11 Å -1,3.46 Å -1, 5.01 Å -1, 11.4 Å -1
The angle between the incident beam and spectrometer is 50 degree, please estimate the covering range of BZ at 6 eV, 21.2 eV, 50 eV, 100 eV and 500 eV photon energy.Answer: 0.51 Å -1, 1.61 Å -1, 2.65 Å -1, 3.83 Å -1, 8.45 Å -1
The BZ in single layer graphene, the magnitude of ΓK is 1.703 Å -1. If you plan to probe the band structure of graphene near the K-point, what are the required angle between the surface normal and spectrometer at 6 eV, 21.2 eV, 50 eV, 100 eV and 500 eV photon energy?Answer: mission impossible, 54 degree, 29.5 degree, 19.9 degree, 8.6 degree
sin5123.0
)cos(5123.0
//
0
2
kin
kin
Ek
VEk
Lattice constant :Graphene : 2.46 ÅCu(111) : 2.08 ÅMoS2 : 3.12 Å
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S Mathias et al., J. Physics : Conference series (2009)
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You need to understand the crystal structure of solids.
The sample characterization, such as the orientation and crystalline, is quite important before the experiment.
XRD, Laue diffraction and LEED are required.
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Superconducting gap ~ 1 – 100meV
Optical Phonons: ~ 40 - 200 meV
Magnons: ~ 10 meV - 40 meV
Pseudogap ~ 30-300 meV
Multiphonons and multimagnons ~ 50-
500 meV
Orbital fluctuations (originated from
optically forbidden d-d excitations): ~ 100
meV - 1.5 eV
Superconducting gap
Multiphonons/
Multimagnons/
pseudogaps
0
100meV
X
3 eV
1 eV
Mott Gap,C-T Gap
dd excitations,Orbital Waves
Optical Phonons,
Magnons,Local Spin -flips
Energy scale and important excitations
Requirement: High Energy Resolution with High Intensity
Z. Hussain, ALS summer school
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Hufner, Very high resolution photoelectron spectroscopy
Superconducting gap
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Light sources and terminology
• Ultraviolet Photoemission Spectroscopy (UPS)
• UV He lamp (21.2 eV, 40.8 eV)
• Laser : 6 eV (BBO), 8 eV (KBBF), 11 eV (gas cell) or HHG (High harmonic generation)
• Valence band PES, direct electronic state info.
• X-ray Photoemission Spectroscopy (XPS)
(Electron Spectroscopy for Chemical Analysis) (ESCA)
• X-ray gun (Al: 1486.6 eV, Mg: 1253.6 eV)
• core level PE, indirect electronic state info
• chemical analysis
• Synchrotron radiation
• continuous tunable wavelength
• valance band and core level
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Current status of ARPES end station at TLS
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Energy range : 5 eV~120 eVE/ΔE: 100,000 at 16 eV and 64 eVScienta R4000 analyzerManipulator : 6-axis motorized manipulator Sample Preparation: in-situ cleave, thin film growthMeasurement temperature range : 10 K~ 350 KBase pressure : 4.5x10-11 torr
R4000
Load-lock system
Preparation chamber
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Basic principles of electron spectrometers / analyzers
Kyle Shen, IGERT Lecture 2008
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The state-of-the-art in electron spectroscopy
Kyle Shen, IGERT Lecture 2008
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Early ARPES experimental result
Now a 2-D detector with ± 30° and 0.1° angular resolution can be obtained.
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• Angle-resolved spectrometers collects electrons as a function of kinetic energy and emission angle
• Due to the slit, only angles along one axis (qx) can be detected simultaneously
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Lens axis
Slit
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Constant energy mapping for ARPES Scan
• Deflection can also be done in y
• This enables full cone detection, 0<<15, without sample rotation
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Increasing deflection in y
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Angle is the soul of ARPES: Band mapping
Tilt angle scanAzimuthal angle scan
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Experimental geometry
Eli Rotenberg, ALS summer school
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Typical Experimental Result
Accumulate spectra of Rashba effect on Au(111) as the angle is scanned
EDC
MDC
Emission
angle
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Surface state of Au(111)
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Rashba effect on Au(111)
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Deflector analyser
• With the deflector analyser, the electron trajectories can be deflected, to change the range of emission angles that reaches the detector
• Deflection can be done in qx and in qy.
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Graphite
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Ek - θx plane θx - θy plane
Data courtesy : Dr. Yamane, IMS
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The Fermi surface of Bi(111)
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Why are electronsso useful as probesof surfaces?
Or
Not so useful for studying bulk properties !!
Electron Escape Depth : Surface Sensitivity
Minimum due to electron-electron scattering, mainly plasmonsPES is a surface sensitive technique! (requires UHV)High energy photoemission: several keV to increase bulk sensitivity
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The requirement of ARPES
• UHV environment : better than 1x10-
10 Torr
• Single crystals or in-situ growth thin films
• Conductors or semiconductors
• Tunable photon energies
HC Hsu, Ph.D. Thesis NTNU(2010)
Koralek, U. Colorado Ph.D. Thesis (2007)
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Base pressure : 1x10-10 TorrIn-situ cleaved Bi2Se3 single crystal Park et al., PRB (2010)
Single crystals or in-situ growth well-ordered thin films are favorable for ARPES measurement
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Using ARPES to study the electronic structure of 2D materials
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Surface state
Surface states are highly localized in real space, thereforecompletely delocalized in k-space along kz.– NO DISPERSION OF SURFACE STATES in kz direction
Eli Rotenberg, ALS summer school
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Quantum well states
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Absolute coverage of thin films : Ag/Au(111) system
Clean Au(111) LT deposited Ag/Au(111)
Anneal to near RT
Ag S.S
Ag QWs
k|| = 0 normal emissionEDCs
D. A. Luh et. al., PRL (2008)
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Dynamically monitor the thin film growth mechanism
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Binding energy (eV)
0.00.20.40.60.81.01.2
Ph
oto
em
issio
n in
ten
isity (
arb
itra
ry u
nit)
7
813
9
10
11
12
1415
16
17
23
4 5 6
7
16.8 ML
18.2 ML
19.6 ML
21 ML
22.4 ML
23.8 ML
25.2 ML
2.8 ML
4.2 ML
5.6 ML
7 ML
8.4 ML
9.8 ML
11.2 ML
12.6 ML
14 ML
15.4 ML
0 1
Ag coverage (ML)
0 5 10 15 20 25
Bin
din
g e
ne
rgy (
eV
)
0.0
0.2
0.4
0.6
0.8
1.0
C.-M. Cheng et al., APL (2008)
C.-M. Cheng et al.,J. Phys. D: Appl. Phys. (2008)
D.-A. Luh et al., PRB (2008)
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The examination of 2D behavior
63Cheng et al., submitted to PRB
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The examination of 2D behavior : tuning incident photon energy
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2D materials – An OverviewThe most well-known 2D material : Graphene First 2D materials studied in detail. Became famous by the works of Novolesov & Geim since 2004. High mobilities (> 100,000 cm2/Vs at RT) raised expectations in future
electronic devices. Significant attention for 2D materials beyond graphene
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The strictly two-dimensional material
• 70 years ago, Landau argued that strictly 2D crystals were thermodynamically unstable and could not exist
• Before 2004, atomic monolayers only as integral part of 3D structure, grown epitaxially on top of monocrystal
• The discovery of graphene and other free-standing 2D atomic crystals (ex :single layer boron nitride and half-layer BSCCO)
New inroads into low-dimensional physicsNew surprise to provide highly potential for application
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Charge transfer process on ML C60/Cu(111) system
1. Large 7-atom vacancies.2. Significant top Cu layer
coherent distortion.3. Nearly “optimal” C60
3-
doping purely by interface reconstruction.
Ref: W.W. Pai et al., PRL 104, 036103 (2010)
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What Is Graphene
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What is graphene
Very good conductorsExtremely thin and resistant
Zero dimensional: fullerenes
wrapped
One dimensional: carbon nanotubes
Rolled
Three dimensional: graphite
stacked
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How to distinguish the thickness of graphene
Raman spectroscopy
Optical microscopy
A. Ferrari , PRL 97,187401 (2006)
SiO2(200 nm )/Si
B. özyilmaz , NUS, Singapore
Bilayer grapheneSingle layer graphene
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Image : http://infared.lbnl.gov.tw
SLG
Single layer and bilayer graphene
Single layer graphene Bilayer graphene
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Novoselov et al., Nature (2012)
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First treament: graphite
Zhou et al., Nature Physics 2, 595 (2006)
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The experiments in graphene on SiO2 (200nm) and suspended graphene
Knox et al., PRB 78, R201408 (2008)PRB 84, 115401 (2011)
graphite
SLG/SiO2
Graphene on SiO2 Suspended graphene
Suspended graphene
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Multi-thickness domains in an exfoliated graphene
Nano-XPS results on exfoliated graphene samples on SiO2 substrates at the ANTARES beamline, SOLEIL
Avila, Synchrotron Radiation News (2014)
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CVD for large scale graphene film
Kim et al., Nature (2009)
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Graphene formation by decomposition of C60
Perdigao et al., J. Physical Chemistry C (2011)
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Epitaxial growth graphene on SiC
Emtsev et al., PRB (2008)
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The electronic structure of bilayer graphene on SiCsubstrate
Cheng et al., submitted to PRB
TB simulatedExp. at 82 eVData taken at 40 eV
-1.0 eV -1.0 eV
-1.5 eV -1.5 eV
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A intrinsic gap exists or not ?
Novoselov, Nature Mat. (2007)