Experiments with magnetic bottles
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Transcript of Experiments with magnetic bottles
Experiments with magnetic bottles
Melanie MuckeDepartment of Physics and Astronomy
Uppsala University, Sweden([email protected])
outline
part 1: magnetic bottle spectrometer• working principle• layout• features
part 2: synchrotron experiments• coincidences• ICD in water clusters
part 3: FEL experiments• covariance technique with neon• double core holes in hydrocarbons• pump-probe on thymine
part 1: magnetic bottle
Kruit and Read, J. Phys. E 16, 313 (1983): cylindrical poles of electromagnet around interaction region, drift tube with coild around for homogeneous guiding field,detector: MCP + phosphor screen
magnetic bottle – the beginning
e-
e-
strong magnetic field Bi weak magnetic field Bf
qi
vqf
v
z
magnetic bottle - principle
𝜔 𝑖=𝑒𝐵𝑖 /𝑚
𝑟 𝑖=𝑚𝑣 𝑖
𝑒𝐵𝑖
=𝑣 𝑠𝑖𝑛𝜃𝑖 /𝜔𝑖
angular frequency of motion
orbit (cyclotron radius)
angular momentum of circular motion
𝑙𝑖=𝑟 𝑖𝑚𝑣 𝑖=𝑚2𝑣2𝑠𝑖𝑛2𝜃 𝑖
𝑒 𝐵𝑖
Lorentz force
𝐿=𝑒𝑣×𝐵
Bi Bf
qi
vqf
v
magnetic bottle - principle
Bi Bf
qi
vqf
vadiabatic transition
sin𝜃 𝑓
sin 𝜃𝑖
=(𝐵 𝑓
𝐵𝑖
)12
𝑟 𝑓
𝑟 𝑖
=(𝐵𝑖
𝐵 𝑓
)12=𝑀
e.g. Bi = 1 T, Bf = 1 mT qf,max = 1.8°, M = 31.6
𝜔 𝑖=𝑒𝐵𝑖 /𝑚
𝑟 𝑖=𝑚𝑣 𝑖
𝑒𝐵𝑖
=𝑣 𝑠𝑖𝑛𝜃𝑖 /𝜔𝑖
angular frequency of motion
orbit (cyclotron radius)
angular momentum of circular motion
𝑙𝑖=𝑟 𝑖𝑚𝑣 𝑖=𝑚2𝑣2𝑠𝑖𝑛2𝜃 𝑖
𝑒 𝐵𝑖
Lorentz force
𝐿=𝑒𝑣×𝐵
permanent magnetinhomogeneous, strong field (0,4 T)
solenoidhomogeneous, weak field (0,5 mT)
e-
e-
magnetic bottle – as used
replace electromagnet by permanent magnet increase solid angle from 2p to 4p
• time-of-flight spectrometer – cover full kinetic energy range• high transmission over large kinetic energy range• high detection efficiency• capable of multi particle detection
ideally suited to investigate correlation between electrons
magnetic bottle – special features
time of flight spectra need pulsed light source need start signalneed to calibrate
part 2: experiments at BESSY
hn = IR … 10 kV
one electron bunchapprox. 20 mA
d = 76 m
BESSY IIrep. rate 1.25 MHz= 800.5 ns revolution time
synchrotron radiation
magnetic tipmesh
cluster beam flight tube (0.6 m) with homogeneousmagnetic field
detector flange with MCP stack &phosphor screen
joint project with AG Becker, FHI Berlin
experimental setup
B. Hartke, Angew. Chem. Int. Ed. 41, 1468 (2002).
... between molecule and liquid
water clusters
monomer
energies for water follow I. Müller and L. Cederbaum, JCP 125, 204305 (2006).
inner valence
outer valence
core level
continuum
binding energy (eV)
12,85- 19,11
33,37
Intermolecular Coulombic Decay
monomer dimer
12,85- 19,11
33,37
11,91- 19,74
32,59- 34,10inner valence
outer valence
core level
continuum
energies for water follow I. Müller and L. Cederbaum, JCP 125, 204305 (2006).
binding energy (eV)
Intermolecular Coulombic Decay
monomer dimer
12,85- 19,11
33,37
11,91- 19,74
32,59- 34,10
double ionisation potential
„one-site“ 38,63 eV double ionisation potential
„two-site“ 2
7,97 eV
inner valence
outer valence
core level
continuum
energies for water follow I. Müller and L. Cederbaum, JCP 125, 204305 (2006).
binding energy (eV)
Intermolecular Coulombic Decay
I. Müller and L. S. Cederbaum, JCP 125, 204305 (2006).
energy spectrum of the ICD-electron:
calculation for water tetramer
ICD in water clusters
S. Barth et al., JPC A 113, 13519 (2009).
cluster contribution
outer valenceinner valence
photoelectron spectrum of water
outer valenceinner valence
This state can decay via ICD.
+ ICD electrons
S. Barth et al., JPC A 113, 13519 (2009).
cluster contribution
photoelectron spectrum of water
investigate coincident electron pairs
electrons undistinguishable sort by flighttime
slow
fast
flight time electron 2
flight time electron 1
electron-electron coincidence measurement
neon tof-map
flight time electron 2
flight time electron 1
flight time electron 2
flight time electron 2
0
2
0
Ett
DE
time-to-energy conversion
tof map energy map
flight time e2
flig
ht ti
me
e1
kinetic energy e2
kin
etic
en
ergy
e1
hn = 45 eV
coincidence maps of water
expected range for water ICD
energy spectrum shows ICD
qualitative agreement with theoretical spectrum0
hn = 45 eV<N> = 40
ICD spectrum
energy spectrum of the primary electrons vs. kinetic energy
0
spectrum of the intermediate state
hn = 45 eV<N> = 40
coincident intensity vs. binding energy of the final state
DIP H2O monomer
0
spectrum of the final state
hn = 45 eV<N> = 40
• ICD feature shifts with photon energy
• energy of the ICD electron follows the theoretical predictions
M. Mucke et al., Nature Phys. 6, 143 (2010)
variation of the excitation energy
hn = 60 eV<N> = 200
monomercluster
no ICD in the monomer
M. Mucke et al., Nature Phys. 6, 143 (2010)
LCLS startinjector
Experiment and UV laser
~1500 m
part 3: experiments at the LCLS
large collaborations at LCLS
Uppsala UniversityM. MuckeV. ZhaunerchykM. KaminskaM.N. PiancastelliJ.H.D. Eland (also Oxford University)R. Feifel
Stockholm UniversityP. SalénP. v.d.MeulenP. LinussonR.D. ThomasM. Larsson
Imperial College LondonR.J. Squibb (now Uppsala University)M. SianoL.J. Frasinski
ELETTRA TriesteR. RichterK.C. Prince
SLACR. CoffeeM. GlowniaJ. CryanM. MesserschmidtS. SchorbC. BostedtJ. Bozek
Michigan UniversityT. OsipovL. FangB. MurphyN. Berrah
Hiroshima UniversityO. TakahashiS. Wada
Tohoku University, SendaiK. MotomuraS. MondalK. Ueda
MPI, HeidelbergL. FoucarJ. Ullrich
a new bottle...
experiments at the LCLS
AMO hutchHigh Field Physics chamberAug/Sep 2011
FEL beamspectrometer axis
sample beam
rep. rate 120 Hz
magnet
solenoid
FEL sample MCP
e-
e-
pulse parameters
trigger
from FEL
digitiser
online display
experimental set-up
covariance analysis
• difference in correlated and uncorrelated products of electron signals X and Y at two kinetic energies:
C(X,Y) = <XY> - <X><Y>
• jitter corretion (photon energy fluctuation)• partial covariance corrects for intensity fluctuations
of FEL: Cp(X,Y;I) = C(X,Y) - C(X,I)C(I,Y)/C(I,I)
• conditional covariance: groupwise analysis of data from shots of similar intensity
L.F. Frasinski et al., J. El. Spec. Rel. Phenom. 79, 367 (1996).
V. Zhaunerchuk et al., Phys. Rev. A 89, 053418 (2014).
L.F. Frasinski et al., Science 246, 1029 (1989).
Double Core Holes
at the same atomss DCH
at different atomsts DCH
creation of two core holes in a molecule by photon impact
high sensitivity to chemical environment
increased orbital relaxation effect
from L.S. Cederbaum et al., Chem. Phys. 85, 6513 (1986).
recent studies on DCHs
J.H.D. Eland et al., Phys. Rev. Lett. 105, 213005 (2010),P. Lablanquie et al., Phys. Rev. Lett. 106, 063003 (2011),P. Linusson et al., Phys. Rev. A 83, 022506 (2011),P. Lablanquie et al., Phys. Rev. Lett. 107, 193004 (2011),M. Nakano et al., Phys. Rev. Lett. 110, 163001 (2013),L. Hedin et al., J. Chem. Phys., submitted (2013).
synchrotron radiation + multi-particle coincidence
CH4
NH3
C 1s-2
N 1s-2
FEL + single-electron detection
L. Fang et al., Phys. Rev. Lett. 105, 083005 (2010),J. Cryan et al., Phys. Rev. Lett 105, 083004 (2010),N. Berrah et al., PNAS 108, 16912 (2011),P. Salén et al., Phys. Rev. Lett. 108, 153003 (2012),M. Larsson et al., J. Phys. B 46, 164034 (2013).
study of DCHs at FELs
use efficient electron spectrometer, employ covariance technique make up for low repetition rate of FEL pulses by • allowing for multiple ionisation events per light pulse • using a spectrometer of high detection efficiency • being able to handle multiple electrons per ionisation
event
study of DCHs at FELs
”core hole clock”: FEL pulse length vs. core hole lifetime get information on ionisation dynamics
use efficient electron spectrometer, employ covariance technique make up for low repetition rate of FEL pulses by • allowing for multiple ionisation events per light pulse • using a spectrometer of high detection efficiency • being able to handle multiple electrons per ionisation
event
neon: ionisation processes
photon energy 1062 eV
neon: covariance map core-region
FEL parameters40 pC charge mode0.35 mJ pulse energy≤ 10 fs pulse length1062 eV photon energy
neon: covariance map correctiondi
scim
inat
ed d
ata
jitter
cor
rect
ed
raw
dat
a
V. Z
haun
erch
yk, M
. Muc
ke,…
, and
R. F
eife
l, J.
Phys
. B 4
6, 1
6403
4 (2
013)
.
Four
ier d
econ
volu
tion
neon: coincidence vs. covariance
coincidence
V. Zhaunerchyk, M. Mucke, et al., J. Phys. B 46, 164034 (2013).
covariance
neon: covariance map core-region
FEL parameters40 pC charge mode0.35 mJ pulse energy≤ 10 fs pulse length1062 eV photon energy
neon: covariance map core-region
1
3
24
6au
toco
rrela
tion li
ne
5
FEL parameters40 pC charge mode0.35 mJ pulse energy≤ 10 fs pulse length1062 eV photon energy
1 PAP2 PP or PAPAP3 PAPVP, PPVAP or PAPsat
4 PAPAP5 DKV
6 DKVAP
neon: covariance maps
1
3
24
6au
toco
rrelat
ion lin
e
5
7
8
7 PVP8 PAPVP or PPVAP
L.J. Frasinski et al., Phys. Rev. Lett. 111, 073002 (2013), V. Zhaunerchyk et al., J. Phys. B 46, 164034 (2013).
first time distinguish PPV from PVP
1
3
24
6au
toco
rrela
tion li
ne
5
1 PAP2 PP or PAPAP3 PAPVP, PPVAP or PAPsat
4 PAPAP5 DKV
6 DKVAP
core-core region core-valence region
Double Core Holes in hydrocarbons
These slides have been deleted since the results are not yet published.If you want information on the outcomes of our investigation of double core hole states in hydrocarbons (C2H2 and C2H6) at the LCLS, please contact me ([email protected]).
summary on Double Core Holes
• 2dim covariance well suited for analysis of data from low repetition-rate light sources (handling of multiple ionisation events per light shot possible)
• identification of new few-photon processes by electron kinetic energies and comparison of intensity dependency of electron-pair features
• clear signatures for DCHs
Dt
ultrafast processes in thymine
... investigated by pump-probe spectroscopy
UV pump + XFEL probemagnetic bottleAuger difference spectra
Nora Berrah, WMUChristoph Bostedt, LCLS SLACJohn Bozek, LCLS SLACPhil Bucksbaum, PULSE SLACRyan Coffee, LCLSJames Cryan, PULSE SLAC Li Fang, WMUJoe Farrell, PULSE SLACRaimund Feifel, Uppsala UniversityKelly Gaffney, PULSE SLACMike Glownia, PULSE SLACMarkus Guehr, PULSE SLAC, SpokespersonTodd Martinez, PULSE SLAC,Brian McFarland, PULSE SLAC
Shungo Miyabe, PULSE SLACMelanie Mucke, Uppsala UniversityBrendan Murphy, WMU Adi Natan, PULSE SLACTimur Osipov, WMUVladimir Petrovic, PULSE SLACSebastian Schorb, LCLS SLAC Thomas Schultz, MBI, BerlinLimor Spector, PULSE SLACFrancesco Tarantelli, Univ. PerugiaIan Tenney, PULSE SLAC Song Wang, PULSE SLACBill White, LCLS SLACJames White, PULSE SLAC
Early Career GrantReference: McFarland et al. Nature Comm. 5, 4235 (2014)
thymine collaboration
pp*np*
Reaction coordinate
UV
pum
p
Groundstate
Pote
ntial
ene
rgy
np*
n
p
*pGS->pp*
4.5
eV Barrier?
Asturiol et al., J. Phys. Chem. A,113, 10211 (2009)Hudock et al., J. Phys. Chem. A,111, 85 (2007)
competing processes
pp*
np*
Reaction coordinate
Pote
ntial
ene
rgy
CICI
Neutralstates
UV
pum
p
Core ionizedstates
Dicationicstates
SXR
prob
e
Auge
r dec
ayE ki
n
Barrier?
Groundstate
GS
n
p
*pIP
Oxygen 1s
GS->pp*
UV
pum
pX-ray probe Auger decayUV pump
SXR
prob
e
Delay
Electr. Relax.
E kin
np*
Electr. R
elax.
O
O
pump-probe scheme
UV Pump Off UV Pump On
p* Auger Electrons
Difference signal: UV On-UV Off
Auger difference spectra
UV pump: 266 nmXFEL probe: 570 eVretardation 470 V
kinetic energy [eV]
Auger difference spectra
UV Pump Off UV Pump On
p* Auger Electrons
Difference signal: UV On-UV Off
III
III
kinetic energy [eV]
dela
y [p
s]
min
III
dela
y [p
s]de
lay
[ps]
McFarland et al, Nature Comm. 5, 4235 (2014)
IIII II
blue-shift of Auger lines
III
III
kinetic energy [eV]
dela
y [p
s]
min
III
dela
y [p
s]de
lay
[ps]
pp*np*
Reaction coordinate
UV
pum
p
Groundstate
Pote
ntial
ene
rgy
McFarland et al, Nature Comm. 5, 4235 (2014)
IIII II
min
blue-shift of Auger lines
54
III
III
kinetic energy [eV]
dela
y [p
s]
III
dela
y [p
s]de
lay
[ps]
pp*np*
Reaction coordinate
UV
pum
p
Groundstate
Pote
ntial
ene
rgy
min
McFarland et al, Nature Comm. 5, 4235 (2014)
IIII II
no barrier observed
the end
magnetic bottle spectrometer –versatile tool for detection of electrons,especially suitable for correlation studies