Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of...
Transcript of Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of...
![Page 1: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/1.jpg)
Peter Puschnig, APS March Meeting, Boston 2012
Motivation
Orbital tomography:Deconvoluting photoemission spectra of organic molecules
Austria Austria Germany Austrian Science FundP23190-N16
![Page 2: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/2.jpg)
ARPES of PTCDA / Ag(110)ARPES of PTCDA / Ag(110)
Peter Puschnig, APS March Meeting, Boston 2012
Glöckler et al,Surf. Sci. 405, 1-20 (1998).STM
Slide 1
![Page 3: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/3.jpg)
Identifying OrbitalsIdentifying Orbitals
Slide 2Peter Puschnig, APS March Meeting, Boston 2012
![Page 4: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/4.jpg)
Identifying OrbitalsIdentifying Orbitals
Self-interactioncorrected functional
Peter Puschnig, APS March Meeting, Boston 2012 Slide 3
![Page 5: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/5.jpg)
ARPES of PTCDA / Ag(110)ARPES of PTCDA / Ag(110)
Peter Puschnig, APS March Meeting, Boston 2012
Glöckler et al,Surf. Sci. 405, 1-20 (1998).STM
Slide 1
![Page 6: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/6.jpg)
Photoemission IntensityPhotoemission Intensity
One Step Model
Peter Puschnig, APS March Meeting, Boston 2012 Slide 4
![Page 7: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/7.jpg)
Photoemission IntensityPhotoemission Intensity
molecular orbital
One Step Model
Peter Puschnig, APS March Meeting, Boston 2012 Slide 4
![Page 8: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/8.jpg)
Photoemission IntensityPhotoemission Intensity
[Feibelman and Eastman, Phys. Rev. B 10, 4932 (1974).]
Approximation: final state = plane wave
Fourier Transform of Initial State Orbital
plane wave ei k r
One Step Model
molecular orbital
Peter Puschnig, APS March Meeting, Boston 2012 Slide 4
![Page 9: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/9.jpg)
Comparison with DFTComparison with DFT
Molecular Orbitalin Real Space
Calculation ofthe Fourier Transform kx (1/Å)
Hemispherical Cut Through3D Fourier Transform
x
kx (1/Å)
k y (
1/Å
)
kz (1/Å
)
y
z
Peter Puschnig, APS March Meeting, Boston 2012
ky (1/Å
)
Slide 5
![Page 10: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/10.jpg)
Peter Puschnig, APS March Meeting, Boston 2012 Slide 6
The Toroidal Electron Spectrometer for Angle-Resolved Photoelectron Spectroscopy with Synchrotron Radiation at BESSY II
Toroidal Electron Energy AnalyzerToroidal Electron Energy Analyzer
![Page 11: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/11.jpg)
HOMO and Filled LUMOHOMO and Filled LUMO
Puschnig et al. PRB 84, 235427 (2011), Ziroff et al., PRL 104, 233004 (2010).
Peter Puschnig, APS March Meeting, Boston 2012
M1=FLUMO
M2=HOMO
Slide 6
![Page 12: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/12.jpg)
What is the nature of M3?What is the nature of M3?
M2=HOMO
M1=FLUMO
?
Peter Puschnig, APS March Meeting, Boston 2012 Slide 7
![Page 13: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/13.jpg)
ARPES Data-CubeARPES Data-Cube
Peter Puschnig, APS March Meeting, Boston 2012 Slide 8
Eb
kx
ky
![Page 14: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/14.jpg)
ππ -„bands“ of PTCDA-„bands“ of PTCDA
Peter Puschnig, APS March Meeting, Boston 2012 Slide 9
![Page 15: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/15.jpg)
What is the Origin of M3?What is the Origin of M3?
Peter Puschnig, APS March Meeting, Boston 2012
E C F
Slide 10
![Page 16: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/16.jpg)
What is the Origin of M3?What is the Origin of M3?
Peter Puschnig, APS March Meeting, Boston 2012
E C F
Puschnig et al. PRB 84, 235427 (2011), see also: Dauth et al., PRL 107, 193002 (2011).
Slide 11
![Page 17: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/17.jpg)
Projected DOS from ARPES!Projected DOS from ARPES!
Peter Puschnig, APS March Meeting, Boston 2012
C
D
E
F
-3.8 -3.6 -3.4 -3.2 -3.0 -2.8
Eb (eV)
measuredphotemission
data cube
calculatedorbitals
Fit parameters= PDOS
Slide 12
![Page 18: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/18.jpg)
Benchmark for TheoryBenchmark for Theory
Peter Puschnig, APS March Meeting, Boston 2012
C
D
E
F
Slide 13
[1-1
0]
Ag-
row
dire
ctio
n
![Page 19: Orbital tomography: Deconvoluting photoemission spectra of ...pep/P23190-N16/pdf/... · ARPES of PTCDA / Ag(110) Peter Puschnig, APS March Meeting, Boston 2012 Glöckler et al, STM](https://reader036.fdocuments.us/reader036/viewer/2022070912/5fb3ae12c0c8ae0a490ad2c4/html5/thumbnails/19.jpg)
ConclusionConclusion
Peter Puschnig, APS March Meeting, Boston 2012 Slide 14
Orbital Tomography● Make use of characteristic momentum space patterns● Unambiguous identification of molecular features● Density of states projected onto molecular orbitals● Deconvolution beyond limits of energy resolution
Other ApplicationsReal space reconstruction of molecular orbital densities
Puschnig et al., Science 326, 702 (2009).
Hybridization of molecular orbitals mit metallic states
Ziroff et al., Phys. Rev. Lett. 104, 233004 (2010).
Berkebile et al., Phys. Chem. Chem. Phys. 13, 3604 (2011).