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Interactions of charged particles with graphene Zoran Miskovic Department of Applied Mathematics University of Waterloo, Ontario, Canada University of Waterloo: F. Goodman D. Mowbray J. Zuloaga M. Ghaznavi K. Allison Dalian University of Technology, China: Y.-N. Wang Y.-H. Song D.-P. Zhou Collaborators: Vinca Institute, Belgrade, Serbia: Lj. Hadzievski N. Bibic I. Radovic D. Borka V. Borka Jovanovic Support: Centro Atomico Bariloche, Argentina: N. Arista J. Gervasoni S. Segui

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Page 1: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Interactions of charged particles with graphene

Zoran MiskovicDepartment of Applied Mathematics

University of Waterloo, Ontario, Canada

University of Waterloo:

F. GoodmanD. MowbrayJ. ZuloagaM. GhaznaviK. Allison

Dalian University of Technology, China:

Y.-N. WangY.-H. SongD.-P. Zhou

Collaborators:

Vinca Institute, Belgrade, Serbia:

Lj. HadzievskiN. BibicI. RadovicD. BorkaV. Borka Jovanovic

Support:

Centro AtomicoBariloche, Argentina:

N. AristaJ. GervasoniS. Segui

Page 2: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

IntroductionIon interactions with graphene

• Nonlinear screening• Image potential• Stopping force• Wake effectPlasmon excitations by electron beams

• HREELS, energy E~20 eV, substrate phonons• EELS, energy E~100 keV, layered electron gasOutlook

Outline

Page 3: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

graphene

Fullerene, C60 nanotube, CNT graphite, HOPG

Graphene as building block of carbon nanostructures

Page 4: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

• Physical properties:– Electrical, mechanical, thermal– Dependent on: molecular structure,

dielectric environment, local modification• Applications:

– Nanoelectronic devices– Biochemical sensors– New composite materials– Ion storage (H, Li)– Nanoelectromechanical systems (NEMS)

Why study carbon nanostructures ?

Page 5: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Electrons• EELS in STEM: plasmon excitations of σ and π

electrons in CNTs & graphene• HREELS: plasmon excitations of π electrons in

graphene• image potential states: CNTs & grapheneIons

• ion channeling in CNTs• grazing scattering of ions on graphene• friction forces on slowly moving ions• static screening of charged impurities

Electronic response to external charged particles (regime of electronic stopping for moving charges)

Page 6: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

σ*

σ π

π*

Dirac point

low-energy excitationsinvolve π bands only

Band structure

πσ

Electronic structure of graphene

Page 7: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Ambipolar electric field effect in single-layer graphene on top of an oxidized Si wafer

gV+ + + + + + + ++ + + + + + + + + + ++ + +

-- -- ---- -- ----

SiO2

Applying gate potential Vg shifts Fermi energy EF above/below Dirac point (electron or hole doping)

Equilibrium charge carrier density vschemical potential μ may be >0 and <0

, Fermi speed:Linear DOS:

Page 8: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

500 eV Ne+

Ion bombardment vs ion adsorption on grapheneJ.H. Chen et al., Phys. Rev. Lett. (2009), Nature Phys. (2008)

++ + +++

Page 9: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Nonlinear screening of external charge by grapheneM. Ghaznavi et al. Phys. Rev. B 81 (2010) 085416

gV

+ + + + + + + ++ + + + + + + + + + ++ + +

-- -- ---- -- ----

SiO2

hz0

+ Study several effects:• doping via gate potential• finite temperature• exchange interaction effects• distance z0 from graphene• size of gap h to the substrate

Page 10: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

graphene on SiO2(nonlinear results)

graphene on SiO2(linear TF and RPA)

free graphene(linear TF and RPA)

free graphene(nonlinear results)

Screened potential in graphene due to external chargeM. Ghaznavi et al. Phys. Rev. B 81 (2010) 085416

Friedel oscillations

Page 11: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

0 r

0 r

Page 12: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Nonlinear image interaction for external chargeM. Ghaznavi et al. Phys. Rev. B 81 (2010) 085416

Observation of image potential states on epitaxial graphene:S. Bose et al. New J. Phys.12 (2010) 023028

Nonlinear image potential

Page 13: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Interaction of moving external charge with grapheneK.F. Allison et al.,Phys. Rev. 80 (2009), Nanotechnology 21 (2010) 134017

Dielectric function of graphene + substrate: Random Phase Approximation

Study several effects:

• doping via gate potential• damping via Mermin approach• local field effects• phonons in polar substrate• size of gap to the substrate

Stopping force Image force

++

Єsub(ω)

Page 14: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Inter-band single-particle excitations

graphene

2D electron gas (2DEG) with paraboloc band

Loss Function for graphene and 2DEG

Intra-band single-particle excitations

Inter-bandSPEs

Intra-band SPEs

Intra-band SPEs

Page 15: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Stopping and image forces on a point charge moving over epitaxial graphene on SiC and 2DEG (Ag on Si)

Stopping force vs. speed Image force (normalized) vs. distance

graphene

graphene

2DEG

2DEG

2DEG

graphene

graphene

2DEG

2DEG

2DEG

Page 16: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Wake effect due to charge moving at speed v = 4vFand distance z0 = 20 Å from free graphene & 2DEG

with doping equilibrium density n = 1013 cm-2

Fermi wavenumber in graphene:

Page 17: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

HREEL spectra for graphene on a substrateK.F. Allison et al., Nanotechnology 21 (2010) 134017

Total energy loss:

Projectile structure factor:

Surface dielectric function:

Loss function

substrate

graphene

trajectory E = 20 eV

Page 18: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Plasmon coupling with substrate phonon

HREELS spectra for graphene on SiC, exper. by Liu et al. PRB 78 (2008) 201403

Page 19: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Stopping and image forces on projectile moving over graphene on SiC: effects of substrate phonons

CEPAS proceedings

Stopping

Image

Wake potential

V tot(x-vt,y=0,z=0)*z 0/(Ze)

Page 20: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

EEL spectra for free-standing N-layer grapheneexperiment by: T. Eberlein et al., Phys. Rev. B 77 (2008) 233406

d

Electron trajectory

E = 100 keV

σ+πplasmon

πplasmon

Page 21: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Two-fluid, 2D hydrodynamic model for σ and πelectrons: used in single-wall carbon nanotube

experiment: Kramberger et al., Phys. Rev. Lett. 100 (2008) 196803theory: Mowbray et al., Phys. Rev. B 82 (2010) 035405

Plasmon dispersions vs kwith angular mode m for nanotube radius a = 7 Å

ExperimentalEEL spectra

Page 22: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

EELS for free-standing graphite (N >> 1)F. Carbone et al., Chem. Phys. Lett. 468 (2009) 107

Laserexcitationregion

σ+π“bulk”

plasmon

σ+π“surface”plasmon

πplasmon

experiment

model

Page 23: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Outlook

• Electronic energy loss and image interaction important for charged particle interactions with C-nanostructures: energy deposition & transport

• Plasmon excitations in HREELS and EELS: full theory needed for dielectric response of both σ and π electrons

• Ion charge states during scattering need to be considered

• Effects of dielectric environment, particularly substrate phonons

• Concept of friction and screening or mobile ions in aqueous solution

Page 24: Interactions of charged particles with graphenezmiskovi/Miskovic_talk_CEPAS.pdf · • Electronic energy loss and image interaction important for charged particle interactions with

Thank you for your attention