Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the...

42
Determining Parameters in the Spicer- Model and Predicted Maximum QE John Smedley

Transcript of Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the...

Page 1: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Determining Parameters in the Spicer-Model and Predicted Maximum QE

John Smedley

Page 2: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Much of this talk comes from a course on Cathode Physics Matt Poelker and I taught at the US Particle Accelerator School http://uspas.fnal.gov/materials/12UTA/UTA_Cathode.shtml

Reference Material

Great Surface Science Resource: http://www.philiphofmann.net/surflec3/index.html

Modern Theory and Applications of Photocathodes W.E. Spicer & A. Herrera-Gómez

SAC-PUB-6306 (1993)

Page 3: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Electronic structure of Materials •  In an atom, electrons are bound in states of defined energy •  In a molecule, these states are split into rotation and

vibration levels, allowing the valence electrons to have a range of discrete values

•  In a solid, these levels merge, forming bands of allowed energies, with gaps between them. In general these bands confine both the energy and linear momentum of the electrons. These bands have an Electron Density of States (EDoS) that governs the probability of electron transitions.

•  For now, we will be concerned with the energy DoS, and not worry about momentum. For single crystal cathodes (GaAs, Diamond), the momentum states are also important.

•  Calculated using a number of methods: Tight binding, Density functional theory. Measured using photoemission spectroscopy.

Page 4: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

ü

DOS Examples •  For a free electron gas in 3

dimensions, with the “particle in a box” problem gives:

•  For periodic boundary conditions:

•  The number of states in a sphere in k-space goes as V ∝ k3

•  The Density of States (states/eV) is then ∝ V/E ∝ E1/2

•  This is good for simple metals, but fails for transition metals

http://mits.nims.go.jp/matnavi/

ü

X

E= ℏ2k2 /2m = (ℏ2 /2m) (kx2+ky

2+kz2)

kx= (2π/L) nx; nx=0,± 1,± 2,± 3,…

Page 5: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

•  As fermions, electrons obey the Pauli exclusion principle. Thus the energy distribution of occupied states (DOS) is given by the Fermi-Dirac (F-D) function,

•  The temperature dependence of this distribution is typically not important for field emission and photoemission, but is critical for thermionic emission

•  For T=0, this leads to full occupancy of all states below EF and zero occupancy for all states above EF

Occupancy: the Fermi-Dirac Distribution

Page 6: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Surface Barrier •  The work function is the energy required to extract an

electron from the surface •  This has two parts, the electrostatic potential binding the

electrons in the bulk, and the surface dipole which occurs due to “spill-out” electrons

http://www.philiphofmann.net/surflec3/surflec015.html#toc36

Φ = φ(+∞)−µ = Δ φ − µ. surface

bulk

Page 7: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Surface Barrier •  This surface dipole portion can

be modified by adsorbates •  We use alkali metals to reduce

the workfunction of cathodes –  Cs on Ag –  Cs on W –  Cs-O on GaAs

•  Adsorbates can also raise φ –  This is the motivation behind laser

cleaning of metal cathodes

•  Note that different faces of a crystal can have different surface dipoles, and therefore different workfunctions Workfunctions of metals have values between about 1.5 eV and 5.5 eV.

Workfunction change upon the adsorption of K on W(110) R. Blaszczyszyn et al, Surf. Sci. 51, 396 (1975).

Page 8: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Energy

Medium Vacuum

Φ

Vacuum level

Filled States Em

pty States

1)  Excitation of e- in metal Reflection (angle dependence) Energy distribution of excited e-

2) Transit to the Surface e--e- scattering Direction of travel 3) Escape surface Overcome Workfunction Reduction of Φ due to applied

field (Schottky Effect)

Integrate product of probabilities over all electron energies capable of escape to obtain Quantum Efficiency Laser

Φ

Φ’

Krolikowski and Spicer, Phys. Rev. 185 882 (1969) M. Cardona and L. Ley: Photoemission in Solids 1, (Springer-Verlag, 1978)

Three Step Model of Photoemission in Metal

Page 9: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

The opt ical skin depth depends upon wavelength and is given by,

where k is the imaginary part of the complex index of refraction,

and λ is the free space photon wavelength.

Step 1: Absorption of Photon

180 200 220 240 260 280 300100

110

120

130

140

150

Wavelength (nm)

Opt

ical

Abs

orpt

ion

Leng

th (a

ngst

rom

s)

Optical absorption length and reflectivity of copper

The reflectivity is given by the Fresnel relation in terms of the real part of the index of refraction,

kopt πλ

λ4

=

ikn +=η

)),(),((tyReflectivi 21 innR θωω=

0.30 0.31 0.32 0.33 0.34 0.35 0.36 0.37 0.38 0.39 0.40

180 200 220 240 260 280 300

Ref

lect

ivity

Wavelength (nm)

Page 10: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

∫−

+

+=

f

f

E

E

dEENEN

ENENEP

ω

ω

ωω

')'()'(

)()(),(

Probability of absorption and electron excitation:

Step 1 – Absorption and Excitation

•  N(E) is the Density of states. The above assumes T=0, so N(E) is the density of filled states capable of absorbing, and N(E+ω) is the density of empty states for the electron to be excited into.

•  Only energy conservation invoked, conservation of k vector is not an important selection rule (phonon scattering and polycrystalline)

•  We assume the matrix element connecting the initial and final state is constant (not energy dependent)

Iab/I = (1-R) Fraction of light absorbed:

Page 11: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

W.E. Pickett and P.B. Allen; Phy. Letters 48A, 91 (1974)

Lead Density of States

0

0.2

0.4

0.6

0.8

1

1.2

0 2 4 6 8 10 12eV

N/e

V

Efermi Threshold Energy

Nb Density of States

00.5

11.5

22.5

33.5

44.5

0 2 4 6 8 10 12

eV

N/e

V

Efermi Threshold Energy

NRL Electronic Structures Database

Density  of  States  for  Nb  Large  number  of  empty  conduc7on  

band  states  promotes  unproduc7ve  absorp7on  

Density  of  States  for  Lead  Pb  6p  valance  states  

Lack  of  states  below  1  eV  limits  unproduc7ve  absorp7on  at  higher  photon  energies  

Page 12: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Step 2 – Probability of reaching the surface w/o e--e- scattering

•  e- mean free path can be calculated –  Extrapolation from measured values –  From excited electron lifetime (2 photon PE spectroscopy) –  Comparison to similar materials

•  Assumptions –  Energy loss dominated by e-e scattering –  Only unscattered electrons can escape –  Electrons must be incident on the surface at nearly normal

incidence => Correction factor C(E,v,θ) = 1

),,()()(1)()(

),,( θωωλωλ

ωλωλθω EC

EE

EFphe

pheee

++

+=−

kph πλ

λ4

=

Page 13: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Step 2 – Probability of reaching the surface w/o e--e- scattering

•  In the near-threshold regime, an e--e- event is unlikely to leave either electron with energy sufficient to escape –  Treat scattering as a loss mechanism –  Can ignore other scattering mechanisms

•  Assume the probability, S, of an excited electron of energy E > Ef interacting with a valence electron of energy E0 < Ef and imparting energy ΔE is proportional to: –  The number of electrons, N(E0), with energy E0. –  The number of empty states, N(E0 + ΔE), with energy E0 + ΔE. –  The number of empty states, N(E – ΔE) with energy E – ΔE.

•  Again, we assume the matrix elements connecting these states are not energy dependent, so that the probability depends only on the DoS

S(E,E0,ΔE) ∝ N(E0) N(E0 + ΔE) N(E – ΔE)

Page 14: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Step 2 – Probability of reaching the surface w/o e--e- scattering

To obtain the total probability of scattering for an electron of energy E by an electron of energy E0, we must integrate over all possible energy transfers, ΔE:

S(E,E0) ∝

The total scattering probability of an excited electron is

obtained by integrating over all possible “valence” electron energies, yielding

S(E) ∝

The lower limit of integration represents the kinematic

limitation that E + E0 ≥ 2Ef.

⌡⌠

Ef – E0

E – Ef

d(ΔE) N(E0) N(E – ΔE) N(E0 + ΔE)

⌡⌠

2Ef – E

Ef

dE0 ⌡⌠

Ef – E0

E – Ef

d(ΔE) N(E0) N(E – ΔE) N(E0 + ΔE)

Page 15: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Step 2 – Probability of reaching the surface w/o e--e- scattering

The lifetime of the excited state, τ(E), is inversely proportional to this scattering probability: τ(E) ∝ 1/S(E)

The scattering length, λe(E), is related to the lifetime by the velocity. We assume a free electron-like velocity, using Ef as the zero of energy for metals and the bottom of the conduction band for semiconductors:

λe(E) = ν(E) τ(E) = λ0 is a constant that is chosen so that the e-e scattering

length (the length over which the intensity of unscattered electrons is 1/e of the initial intensity) matches a known value of the electron’s mean free path at a single energy for a given material.

λ0 E – Ef

⌡⌠

2Ef – E

Ef

dE0 ⌡⌠

Ef – E0

E – Ef

d(ΔE) N(E0) N(E – ΔE) N(E0 + ΔE)

Page 16: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Step 2: Transport to the Surface

Fe-e: Probability electron at depth s, absorbs a photon and escapes without scattering.

⎟⎟

⎜⎜

⎛+−

−= eeopts

opt

esf λλ

λ

111)(

ee

optee dssfF

+

== ∫λ

λ1

1)(0

metal vacuum

optse λ/−

s

effeeopteeopt ss

ss eeee λλλλλ /11

// −⎟⎟⎠

⎞⎜⎜⎝

⎛+−

−− == −−

metal vacuum

optse λ/−

s

effeeopteeopt ss

ss eeee λλλλλ /11

// −⎟⎟⎠

⎞⎜⎜⎝

⎛+−

−− == −−

opt

s

s

s

excited

opt

opt

opt e

dse

esPλ

λ

λ

λ /

0

/

1

)(−

∞−

⎟⎟

⎜⎜

⎛−

==

⎟⎟

⎜⎜

⎛+

==

∫ −

ω

φφωλ

λ

ωλ ω

φ

ω

φ

effeff

m

ee

eeE

dE

dEE

eff

eff

1

12)(

)(2/3

0

Assume the electron-electron scattering length can be averaged over energy:

4 5 6 7 8 9 10

20

40

60

80

100

TheoryTanumaKrolikowski & Spicer

Energy above Fermi Level (eV)

e-e

Scat

teri

ng L

engt

h (a

ngst

rom

s)

2/3

')()'( ⎟

⎞⎜⎝

⎛= −− E

EEE mmeeee λλ

Krolikowski & Spicer, 1970

This assumes N(E) = constant (more on this later) Dave uses Fe-e instead of T(E,ω)

Em= Energy at which λ0 is known

Page 17: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Step 2 – Probability of reaching the surface w/o e--e- scattering

)()(1)()(

),(ωλωλ

ωλωλω

phe

pheee E

EEF

++

+=−

The probability that an electron created at a depth d will escape is e-d/λe, and the probability per unit length that a photon is absorbed at depth d is (1/λph) e-d/λph. Integrating the product of these probabilities over all possible values of d, we obtain the fraction of electrons that reach the surface without scattering, Fe-e(E,ω),

Page 18: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Electron Mean Free Path in Lead, Copper and Niobium

0

50

100

150

200

250

2 2.5 3 3.5 4 4.5 5 5.5 6Electron Energy above Fermi Level (eV)

MFP

(Ang

stro

ms)

e in Pb

e in Nb

e in Cu

Threshold Energy for Emission Pb Nb Cu

Page 19: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Electron and Photon Mean Free Path in Lead, Copper and Niobium

0

50

100

150

200

250

2 2.5 3 3.5 4 4.5 5 5.5 6Electron Energy above Fermi Level (eV)

MFP

(Ang

stro

ms)

e in Pb190 nm photon (Pb)e in Nb190 nm photon (Nb)e in Cu190 nm photon (Cu)

Threshold Energy for Emission Pb Nb Cu

Page 20: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Escape criterion:

F

eff

total

normal

EEpp

−+==

ω

φθ

maxcos

θ

While photoemission is regarded quantum mechanical effect due to quantization of photons, emission itself is classical. I.e., electrons do not tunnel through barrier, but classically escape over it. This is analogous to Snell’s law in optics

Step 3: Escape Over the Barrier

θ( )ω+= Emptotal 2

ϕθ cossintotalx pp =

metal vacuum

x

z

y

ϕθ

( )ω+= Emptotal 2

ϕθ cossintotalx pp =

metal vacuum

x

z

y

ϕ

ω+Eφω −−+ FEE

φ+FE

inmax,θ

ω+Eφω −−+ FEE

φ+FE

inmax,θ

 

FEE −+ ω

φ

Page 21: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Step 3 - Escape Probability

•  Criteria for escape:

•  Requires electron trajectory to fall within a cone defined by angle:

•  Fraction of electrons of energy E falling with the cone is given by:

•  For small values of E-ET, this is the dominant factor in determining the emission. For these cases:

•  This gives:

θ φ>= ⊥⊥

mk

mp

22

222

21min )(cos

FEEkk

−+== ⊥

ωφ

θ

∫−+

∝f

f

E

E

dEEDQEωφ

ν

)()(

2)()( φνν −∝ hQE

))(1(21)cos1(

21''sin

41)( 2

1

0

2

0 FEEddED

−+−=−== ∫ ∫ ω

φθϕθθ

π

θ π

Page 22: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

At this point, we have N(E,ω) - the Energy Distribution Curve of the emitted electrons:

EDC(E,ω)=(1-R(ω))P(E,ω)Fe-e(E,ω)D(E) To obtain the QE, integrate over all electron energies capable

of escape: More Generally, including temperature:

∫−+

−−=f

f

E

Eee dEEDEFEPRQE

ωφ

ωωωω

)(),(),())(1()(

EDC and QE

∫ ∫∫

∫ ∫∫∞

Φ+−+

Φ+−+

−=

−+

0

2

0

1

1

2

0

1

)(cos

)(cos)()())(1)((

),,()(cos)()())(1)(( ))(1()( max

π

ωφ

π

θ

θωω

θωθωω

ωω

ddEFENEFENdE

dEFdEFENEFENdERQE FE

eeE

D. H. Dowell et al., Phys. Rev. ST-AB 9, 063502 (2006)

Page 23: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

∫ ∫∫

∫ ∫∫∞

− −

−+

Φ+−+

Φ+−+

−=

ω

π

ωφ

π

θ

θωω

θωθωω

ωω

F

effF

EFDFD

Eee

EFDFD

ddEfENEfENdE

dEFdEfENEfENdE

RQE2

0

1

1

2

0

1

)(cos

)(cos)()())(1)((

),,()(cos)()())(1)((

))(1()( max

Elements of the Three-Step Photoemission Model

Fermi-Dirac distribution at 300degK

schottkyeff φφφ −=TkEEFD BFeEf /)(1

1)(−+

=

0 5 100

0.5

1

1.5

Energy (eV)EF EF+φeff EF+φeff-hω

Bound electrons

EF+hω

hω-φeff

E E+hω

φeff

Emitted electrons

Step 1: Absorption of photon Step 3: Escape over barrier Step 2: Transport to surface

Electrons lose energy by scattering, assume e-e scattering dominates, Fe-e is the probability the electron makes it to the surface without scattering

Escape criterion: effnormal

mp

φ>2

2

θ

)(2 ω+−= Ftotal EEmp

ω

φθ

+−== ⊥

F

eff

total EEpp

maxcos

θω cos)(2 +−= Fnormal EEmp

Photo-Electric Emission

Page 24: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Derivation of QE

∫ ∫∫

∫ ∫∫∞

− −

−+

Φ+−+

Φ+−+

−=

ω

π

ωφ

π

θ

θωω

θωθωω

ωω

F

effF

EFDFD

Eee

EFDFD

ddEfENEfENdE

dEFdEfENEfENdE

RQE 2

0

1

1

2

0

1

)(cos

)(cos)()())(1)((

),,()(cos)()())(1)((

))(1()( max

( ) ( )

∫∫∫

∫∫∫

Φ

Φ

−=

−−

+

+−+

− π

ω

π

ω

φωφ

θ

θ

ωωω2

0

1

1

2

0

1

)(cos

)(cos

)(1)(dddE

dddE

FRQEF

F

efff

F

effF

E

E

EE

E

E

ee

If we assume N(E)=constant, and a approximate F-D with step function since kBT<<EF :

The QE is then given by: ( )

2

2/3

212

1)(2)(

1

)(1)(⎥⎥⎦

⎢⎢⎣

+

+−

+

⎟⎟

⎜⎜

⎛++

−=

ω

φ

ωω

ω

φφω

λ

ωλ

ωω

F

effFF

eff

m

eff

mee

optEEE

EE

RQE

D. H. Dowell, K.K. King, R.E Kirby, J.F. Schmerge and J. Smedley, "In situ cleaning of metal cathodes using a hydrogen beam," PRST-AB 9, 063502 (2006)

TkEEFD BFeEf /)(1

1)(−+

=

0 5 100

0.5

1

1.5

Energy (eV)EF EF+φeffEF+φeff-hω

Bound electrons

EF+hω

hω−φeff

E E+hω

φeff

Emitted electrons

TkEEFD BFeEf /)(1

1)(−+

=

0 5 100

0.5

1

1.5

Energy (eV)EF EF+φeffEF+φeff-hω

Bound electrons

EF+hω

hω−φeff

E E+hω

φeff

hωhω

Emitted electronsState Occupation

Number

State Energy

TkEEFD BFeEf /)(1

1)(−+

=

0 5 100

0.5

1

1.5

Energy (eV)EF EF+φeffEF+φeff-hω

Bound electrons

EF+hω

hω−φeff

E E+hω

φeff

Emitted electrons

TkEEFD BFeEf /)(1

1)(−+

=

0 5 100

0.5

1

1.5

Energy (eV)EF EF+φeffEF+φeff-hω

Bound electrons

EF+hω

hω−φeff

E E+hω

φeff

hωhω

Emitted electronsState Occupation

Number

State Energy

Page 25: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

QE for a metal

( ) ( )

1

2

01 2

1 0

(cos )

( ) 1 ( )(cos )

F

F eff

F eff

F

F

E

EE E

e e E

E

ddE d

QE R Fd ddE

π

ϕϕ ω ω

π

ω

θ

ω ω ωθ

++ − +

−−

Φ

= −

Φ

∫∫ ∫

∫ ∫∫

h h

hStep  1:  Optical  Re.lectivity    ~40%  for  metals    ~10%  for  semi-­‐conductors Optical  Absorption  Depth      ~120  angstroms Fraction  ~  0.6  to  0.9

Step  2:  Transport  to  Surface e-­‐e  scattering  (esp.  for  metals)              ~30  angstroms  for  Cu e-­‐phonon  scattering  (semi-­‐conductors) Fraction    ~  0.2

Step  3:    Escape  over  the  barrier E    is  the  electron  energy EF  is  the  Fermi  Energy φeff    is  the  effective  work  function eff W Schottkyφ φ φ= −

• Sum  over  the  fraction  of  occupied  states  which  are  excited  with  enough  energy  to  escape, Fraction  ~0.04

• Azimuthally  isotropic   emission Fraction  =1

• Fraction  of  electrons  within  max  internal  angle  for  escape,  Fraction  ~0.01

QE ~ 0.5*0.2*0.04*0.01*1 = 4x10-5

Page 26: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

“Prompt”

Metals have very low quantum efficiency, but they are prompt emitters, with fs response times for near-threshold photons:

To escape, an electron must be excited with a momentum vector directed toward the surface, as it must have

The “escape” length verses electron-electron scattering is typically

under 10 nm in the near threshold case. Assuming a typical hot electron velocity of 106 m/s, the escape time is 10 fs.

(this is why the LCLS has a Cu photocathode)

W.F. Krolikowski and W.E. Spicer, Phys. Rev. 185, 882 (1969) D. H. Dowell et al., Phys. Rev. ST Accel. Beams 9, 063502 (2006) T. Srinivasan-Rao et al., PAC97, 2790

φ>⊥

mk2

22

Page 27: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Lead QE vs Photon energy

1.0E-04

1.0E-03

1.0E-02

4.00 4.50 5.00 5.50 6.00 6.50 7.00

Photon energy (eV)

QE

TheoryMeasurement

Vacuum Arc deposited Nb Substrate Deuterium Lamp w/ monochromator 2 nm FWHM bandwidth Phi measured to be 3.91 V

Page 28: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Copper QE vs Photon Energy

1.E-06

1.E-05

1.E-04

1.E-03

1.E-02

4.0 4.5 5.0 5.5 6.0 6.5 7.0Photon energy(eV)

QE

Theory

Dave's Data

D. H. Dowell et al., Phys. Rev. ST-AB 9, 063502 (2006)

Page 29: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Energy

Medium Vacuum

Φ

Vacuum level

Three Step Model of Photoemission - Semiconductors

Filled States Em

pty States

1)  Excitation of e- Reflection, Transmission,

Interference Energy distribution of excited e-

2) Transit to the Surface e--phonon scattering e--defect scattering e--e- scattering Random Walk

3) Escape surface Overcome Workfunction

Multiple tries Need to account for Random Walk in

cathode suggests Monte Carlo modeling

Laser

No States

Page 30: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Cs3Sb (Alkali Antimonides) Work function 2.05 eV, Eg= 1.6 eV Electron-phonon scattering length

~5 nm Loss per collision ~0.1 eV Photon absorption depth

~20-100 nm Thus for 1 eV above threshold, total

path length can be ~500 nm (pessimistic, as many electrons will escape before 100 collisions)

This yields a response time of ~0.6 ps

Alkali Antimonide cathodes have been

used in RF guns to produce electron bunches of 10’s of ps without difficulty

D. H. Dowell et al., Appl. Phys. Lett., 63, 2035 (1993) W.E. Spicer, Phys. Rev., 112, 114 (1958)

Page 31: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Assumptions for K2CsSb Three Step Model •  1D Monte Carlo (implemented in Mathematica) •  e--phonon mean free path (mfp) is constant

–  Note that “e--phonon” is standing in for all “low energy transfer” scattering events

•  Energy transfer in each scattering event is equal to the mean energy transfer

•  Every electron scatters after 1 mfp •  Each scattering event randomizes e- direction of travel •  Every electron that reaches the surface with energy

sufficient to escape escapes •  Cathode and substrate surfaces are optically smooth •  e--e- scattering is ignored (strictly valid only for E<2Egap) •  Band bending at the surface can be ignored •  k-conservation unimportant (uncertainty principle)

Page 32: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Parameters for K2CsSb Three Step Model

•  e--phonon mean free path •  Energy transfer in each scattering event •  Emission threshold (Egap+EA) •  Cathode Thickness •  Substrate material

Parameter estimates from: Spicer and Herrea-Gomez, Modern Theory and

Applications of Photocathodes, SLAC-PUB 6306 Basic Studies of High Performance Multialkali

Photocathodes; C.W. Bates http://www.dtic.mil/dtic/tr/fulltext/u2/a066064.pdf

Page 33: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

A.R.H.F. Ettema and R.A. de Groot, Phys. Rev. B 66, 115102 (2002)

0.0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0.8

0.9

-3 -1 1 3 5 7 9 11

Sta

tes/

eV

eV

K2CsSb DOS

Filled States

Empty States

Band Gap

Page 34: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Unproductive absorption

In “magic window” ω < 2Eg

Onset of e-e scattering

Spectral Response – Bi-alkali

T. Vecchione, et al, Appl. Phys. Lett. 99, 034103 (2011)

Page 35: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Laser Propagation and Interference

2¥10-7 4¥10-7 6¥10-7 8¥10-7 1¥10-6

0.2

0.4

0.6

0.8

Vacuum K2CsSb 200nm

Copper

563 nm

Laser energy in media

Not exponential decay

Calculate the amplitude of the Poynting vector in each media

Page 36: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

QE vs Cathode Thickness

00.05

0.10.15

0.20.25

0.30.35

0.40.45

0.5

2 2.2 2.4 2.6 2.8 3 3.2 3.4photon energy [eV]

QE

50 nm200 nmExperiment20 nm20 nm10 nm

Data from Ghosh & Varma, J. Appl. Phys. 48 4549 (1978)

Monte Carlo for K2CsSb

Page 37: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

QE vs Mean Free Path

0.000.050.100.150.200.250.300.350.400.450.50

2.00 2.20 2.40 2.60 2.80 3.00 3.20 3.40photon energy [eV]

QE

Experiment10 nm mfp5 nm mfp20 nm mfp

Page 38: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Thickness dependence @ 543 nm

0

0.1

0.2

0.3

0.4

0.5

0.6

0.7

0 50 100 150 200 250

Thickness (nm)

Tran

smis

sion

/Ref

lect

ion

0

0.01

0.02

0.03

0.04

0.05

0.06

0.07

0.08

0.09

0.1

QE

ReftransTotal QEQE w/o R&T

Page 39: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Spatial Variation of QE for a Thin K2CsSb Cathode

QE in reflection mode

00.20.40.60.81

1.21.4

465 470 475 480 485 490 495

Position in mm

QE

%

Page 40: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Parameters, and how to affect them Reflectivity depends on angle of incidence and cathode

thickness. Though already small, structuring of the photocathode can further reduce loss due to reflection.

R. Downey, P.D. Townsend, and L. Valberg, phys. stat. sol. (c) 2, 645 (2005)

Page 41: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Parameters, and how to affect them Reflectivity depends on angle of incidence and cathode

thickness. Though already small, structuring of the photocathode can further reduce loss due to reflection.

Increasing the electron MFP will improve the QE. Phonon

scattering cannot be removed, but a more perfect crystal can reduce defect and impurity scattering:

A question to consider: Why can CsI (another ionic crystal,

PEA cathode) achieve QE>80%?

Large band gap and small electron affinity play a role, but, so does crystal quality.

T.H. Di Stefano and W.E. Spicer, Phys. Rev. B 7, 1554 (1973)

R. Downey, P.D. Townsend, and L. Valberg, phys. stat. sol. (c) 2, 645 (2005)

Page 42: Determining Parameters in the Spicer- Model and Predicted ......Determining Parameters in the Spicer-Model and Predicted Maximum QE ... • For a free electron gas in 3 dimensions,

Concluding Thoughts •  As much as possible, it is best to link models to measured

parameters, rather than fitting –  Ideally, measured from the same cathode

•  Whenever possible, QE should be measured and modeled as a function of wavelength. Energy Distribution Curves would be wonderful!

•  Spicer’s Three-Step model well describes photoemission from most metals tested so far, and provides a good framework forsemiconductors

•  The model provides the QE and EDCs, and a Monte Carlo implementation will provide temporal response

•  A program to characterize cathodes is needed, especially for semiconductors (time for Light Sources to help us)

Thank You!