Optical Spectroscopy of Tungsten Carbide

for electron EDM Measurement

Portrait of Edward James Rene Magritte (1937)

Electron with
Non-zero EDM

P-violation

de
1m

Jeongwon Lee
Leanhardt AMO group
Department of Physics, University of Michigan

+
_

Contents
1. Introduction
- what is an electron Electric Dipole Moment (eEDM)?
- eEDM measurement scheme
- advantages of WC molecules

2. Experimental Results
- 1st generation : continuous supersonic beam source
- 2nd generation : pulsed supersonic beam source
3. Uncertainty Analysis
- Systematic uncertainty
- Statistical uncertainty
4. Summary

Contents

1. Introduction

electron EDM violates symmetry

Non-zero electron Electric Dipole Moment

Violates both time (T) and parity (P) reversal symmetry

e- EDM : not detected yet

10-24

Current Experimental Limit :

|de| < 1.05 x 10-27 e*cm [~10-18 Debye]

de [e*cm]

10-28
10-30
10-32

SUSY
Left-Right
Multi-Higgs

10-26

Improving the precision of e-EDM measurement

=> Probe for new physics beyond Standard Model

10-34
10-36
10-38
10-40

Standard Model
Too far from current experimental limit

EDM Measurement Scheme

- Case 1 : E & B Field Parallel
de E

de

mBB

+
_

m 1

mBB

m0

m 1

B E

d eE

Total Shift 1: total,1

2 m m B 2d e E
h

de

EDM Measurement Scheme

- Case 2 : E & B Field anti-Parallel
de E

de

mBB

+
_

m 1

mBB

m0

B E

m 1

de

d eE
Reversing E field relative to B field
=> Stark Shift in opposite direction

de

Total Shift 2: total, 2

vtotal,1 vtotal, 2
4E

2 m m B 2d e E
h

Advantage 1: Large Electric Field

- Heavy Polar Molecule

Effective Electric Field : E-field seen by e- inside

atoms and molecules
Elab

Maximum Elab ~ 105 V/cm

High Z atoms : Eeff ~ 107 V/cm

Upper Limit from Tl expt.[1] : |de| < 1.6 x 10-27 e*cm [~10-18 Debye]

Heavy Polar Molecules : Eeff ~ 1010 V/cm

Upper Limit from YbF expt.[2] : |de| < 1.05 x 10-27 e*cm

[1] B.C. Regan, E.D. Commins, C.J. Schmidt & D. DeMille

[PRL 88, 071805 (2002)]
[2] J.J. Hudson, D.M. Kara, I.J. Smallman, B.E. Sauer, M. R. Tarbutt & E.A. Hinds [Nature 473, 493-496 (2011)]

Advantage 2: Small Magnetic Moment

- 31 state of WC

spin:

S 1
orbital:

Spin & orbital projection

in opposite direction

L2

spin + orbital: L S 1
When gS ~ 2 and gL ~ 1, g ~ 0
Very Small magnetic moment:
measured to be g = 0.022 [1]

[1] F. Wang & T.C. Stemlie, JCP 135 104313 (2011)

Advantage 3: Internal Comagnetometer

- -doublet structure of WC

B Elab

Eeff 0

melElab
m 1

Eeff 0

melElab
m0

melElab

Small doublet splitting (nearly degenerate opposite parity states)

=> Efficient Zeeman Shift Cancellation

m 1

melElab

Contents

2. Experimental Results

WC Molecular
Spectrum
LIF
Spectroscopy
3 transitions per J level.

J=4

[20.6] =2

J=3

R transition : J = +1
Q transition : J = 0
P transition : J = - 1

J=2

v=4
v=3
v=2
v=1
v=0

R(1) line
X 31
J=3
e = 983.2 cm-1
~ 1400 K

v=0

J=2
J=1

B = 0.509 cm-1 ~ 0.7 K

Ro-vibrational ground state => EDM state

Rotational Temperature Requirement

B = 0.509 cm-1 ~ 0.7 K

e = 983.2 cm-1 ~ 1400 K

(Fractional EDM state)

Fractional ro-vibrational
ground state @ 1000 K ~ .001
@ 100 K ~ .01
We want colder molecules!
Most general way of Cooling to
1K level : supersonic expansion

1st generation experiment:

Continuous WC molecular beam apparatus

1. Evaporation
Zone
(Seeding Zone)

3. Optical
Spectroscopy
Zone

2. Differential
Pumping Zone

1. Evaporation Zone
- Seeding Technique
Resistive Heating Method

Tungsten Vapor Pressure

=> 1 X 10-6 Torr at 2700K

Compare with,
Ytterbium Vapor Pressure
=> 7 Torr at 1000K

W CH 4
WC 2H 2

1% molecular formation

184W
182W

183W

186W

WC

1. Evaporation Zone
- Cooling Mechanism
Supersonic Effect

Tungsten Filament (~150W)

(Resistive Heating Method)

Thermalization

E. Conversion

1. Far from the throat of the nozzle, Thermalization process dominates

=> Energy Transfer from W / WC to Buffer gas molecule
2. Closer to the throat, Supersonic Effect dominates
=> Converting thermal energy into direct kinetic motion

Continuous
2. Differential
WC molecular
Pumping
beam
Zone
apparatus
- Pumping Capacity Issue

<Top View>

Too Much Flux is Lost!

Continuous
2. Differential
WC molecular
Pumping
beam
Zone
apparatus
- How to overcome the pumping capacity

<Top View>

25 cm
2cm

Flux regained by
decreasing the
nozzle-skimmer distance

3. Optical Spectroscopy Zone

Tungsten Supersonic Beam Characterization

Radial Probe
@ 384.9nm

Top View
Atomic /
Molecular Beam

Laser Induced Fluorescence

Spectroscopy of Tungsten 5D0 5F1

Side View of
Spectroscopy
Chamber

5F
1

384.9nm

5D
0

(Ground State)

Calculated
Photon
Collection
efficiency
= 0.063

Axial Probe
@ 384.9nm

Flux Separation Technique

- Atom Flux / Radiated Light Flux

Flux passing through nozzle & skimmer (2 apertures)

Filament light background reduced by a factor of 1000,

while the LIF signal decreased only by a factor of 5

Signal to Noise
Increase by factor of 6

ContinuousTungsten
WC molecular
LIF spectrum
beam apparatus
- 1 Torr Argon, 1.5mm Nozzle, 3mm Skimmer

1.8 GHz
(vaxial~681m/s)
260 MHz
(~40K)

<Axial Mach Number>

vaxial

90 MHz
(~0.05 rad)

vaxial
681m / s

10
67m / s
5 k BTtrans
2 mtungsten

at supersonic regime

As for Tungsten Carbide

Tungsten
Signal to Noise

~1200

Tungsten Carbide
Molecular Formation

~1%

Tungsten Carbide
In Rovibrational
Ground State

at 40K,
~5%

(estimated)

Tungsten Carbide
Ground State
Signal to Noise

~0.6

LIF signal of WC molecules was not detected from the continuous beam.
=> 2nd generation pulsed supersonic beam source was developed.

Advantage of pulsed beam

- Diagram of Ideal Case
Time Delay (= time of flight)
Radiated
Light Flux
(Noise)
Atomic
Flux
(Signal)
Photon
Counter
gate

2nd generation experiment:

Pulse WC molecular beam apparatus
Vacuum Pump

PMT
Nd:YAG Laser

Pulse Valve

W + CH4 WC + 2H2

485nm diode laser

350psi
90% Argon
+ 10% CH4

Tungsten Rod

Detect Laser Induced Fluorescence of WC,

75 cm away from the source

WC Molecular
Spectrum
LIF
Spectroscopy

First detected signal !

J=4

[20.6] =2

J=3

N 101 s 1

J=2

v=4
v=3
v=2
v=1
v=0

~10MHz

R(1) line
X 31
J=3
J=2

v=0

J=1

Ro-vibrational ground state => EDM state

Contents

3. Uncertainty Analysis

X31 ground state of WC molecules

Advantages of X31 State WC Molecules for eEDM experiments
B Elab~10V/cm
melElab
calculated
[1]
Eeff~-36GV/cm

m 1

melElab

Large Effective Electric Field

Eeff 0
m0

Eeff 0

melElab
m 1

melElab

Zeeman Shift Cancellation with doublet

Other eEDM experiments with 31 State Molecules: JILA (HfF+ , ThF + ), Harvard/Yale (ThO)
[1] A.N. Petrov & A.V. Titov, private communication

Uncertainties of the Measurement Scheme

Uncertainties of the eEDM measurement scheme with WC

B Elab~10V/cm
melElab
calculated
Eeff~-36GV/cm

gf

m 1

ge

melElab

Large Effective Electric Field

=> how accurate is the calculation?

Eeff 0
m0

Eeff 0

melElab
m 1

melElab

Zeeman Shift Cancellation with doublet

How close are the g factors?
(ge and gf)

Uncertainty Analysis 1
- Effective electric field
Near the heavy nucleus, electric field seen by the electron ( Eeff ) can be written as,

Eeff

Ze
2 rel
a0

Uncertainty in
Eeff field

1
WC | 2 | WC
r

where rel a0 s1 / 2 |
2

Uncertainty in

| WC

r
r

[1]

| p1 / 2

Uncertainty in
Hyperfine constant
measurement
WC | H hyperfine | WC

[1] I.B. Khriplovich & S.K. Lamoreaux, CP violation without Strangeness (1997)

Tungsten Carbide R lines

LIF spectroscopy of R branches of [20.6] =2 <- X 31 (4,0) band system
[20.6] =2
J=4
J=3
J=2

v=4
v=3
v=2
v=1
v=0

R(1) line

R(2) line

X 31

=> Lower J lines have larger splittings

J=3

J=2
v=0

F ( F 1) J ( J 1) I ( I 1)

H Hyperfine h
2
J
(
J

1
)

J=1

Hyperfine Structure of 183W12C

(I = )
a

183W12C

R(1)

F ( F 1) J ( J 1) I ( I 1)

Hyperfine Splitting h
2 J ( J 1)

a
183W12C

R(2)
h1 1171 12MHz
h2 1258 13MHz

(ground)
(excited)

Uncertainty Analysis 1
- Effective electric field
Uncertainty in
Eeff field

Uncertainty in
Hyperfine constant
measurement

Uncertainty in

1
WC | 2 | WC
r

| WC

WC | H hyperfine | WC

Hyperfine measurement as the test of electronic wavefunction near the nucleus

Our expt.

1171 12 MHz

Previous expt.

[1]

1363 51 MHz

Calculated

[2]

1160 MHz
[1] F. Wang & T.C. Stemlie, JCP 134 201106 (2011)
[2] A.N. Petrov & A.V. Titov, private communication

Uncertainty Analysis 2
- Difference in g factors
There is a small difference in g factors (g) between top and bottom doublet.

f e 2m B B( g f ge ) 4de Eeff

melElab
m 1

Systematic Uncertainty 2mB Bg

melElab

Eeff 0

m0
Eeff 0

melElab
m 1

melElab

Summary of relation between

-doublet and g

Smaller -doublet

Smaller Elab to
fully polarized WC

Polarization condition

H doublet me Elab

Smaller g

g( Elab ) me Elab

g
Brotation

Change in Experimental Settings

F ( F 1) J ( J 1) I ( I 1)

H Hyperfine h
2
J
(
J

1
)

Low Trot Preferred

H doublet o~J ( J 1)

Under-expansion &
Higher YAG power

High Trot Preferred

Change in Experimental Settings

- Axial Velocity Distribution
F ( F 1) J ( J 1) I ( I 1)

H Hyperfine h
2
J
(
J

1
)

Low Trot Preferred

Under-expansion &
Higher YAG power

H doublet o~J ( J 1)
High Trot Preferred

Tungsten Carbide Doublet

- Experimental Data
J
(=J+1)
For R
branch

R(4)

R(5)

e/f
f/e
2o~2 ( J 1) J ( J 1)( J 2)

f/e

182W12C

2o~1 J ( J 1)

e/f
Doublet Splitting
2o~1 J ( J 1) 2o~2 ( J 1) J ( J 1)( J 2)

184W12C

Based on fitting,

o~1 418 18 kHz

(previous : 400 13kHz)
o~2 1.1kHz

186W12C
[1]

[1] F. Wang & T.C. Stemlie, JCP 136 044316 (2012)

Systematic Uncertainty from g

Smaller -doublet

o~1 418 18 kHz

Smaller Elab to
fully polarized WC

Smaller g

Elab 10V/cm

g(10V/cm) 3 10-5

Smaller
systematic
uncertainty

Systematic Uncertainty 2m B Bg 100mHz (when B ~ mG)

limits the sensitivity at d e 10-29 e cm level (when E eff ~ 36GV / cm)

Further Suppression of
Systematic Uncertainty from g

Detailed calculation revealed a g-factor crossing point => suppression of systematics as g~0
* J. Lee, J. Chen, L. Skripnikov, A. Petrov, A. Titov, A. Leanhardt, full manuscript in preparation

Further Suppression of
Systematic Uncertainty from g

g-factor crossing point results at Elab = 2V/cm

Need to check whether the molecule is fully polarized

=> Eeff = 0.85 * 36GV/cm when Elab = 2V/cm

* J. Lee, J. Chen, L. Skripnikov, A. Petrov, A. Titov, A. Leanhardt, full manuscript in preparation

Statistical Uncertainty of
Ramsey Spectroscopy
Chop relative direction of E and B and measure frequency difference.
L ~ 1 m, v ~ 300 m/s, t ~ 3 ms
/2

populations
oscillate

/2

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

E B

E B

--------------Frequency Resolution :

1
2t N T

sin2()

ei
cos2()

Statistical Uncertainty of
eEDM measurement
Frequency Resolution :

1
2t N T

Coherence time
(= time of flight)

Rate of EDM state

measurement

Integration time

Beam line extension

Increase of
molecular density

Taking more
measurements
at a fixed rate

Stronger transition

Statistical Uncertainty of
eEDM measurement

EDM Shift :

2d e Eeff
h

VS.

Frequency
Resolution :

Current Status

Future Plan

Eeff

-36GV/cm

-36GV/cm

~1ms

~2ms

N
T

~10 Hz

~104 Hz

1day (~105s)

1day (~105s)

|de| detection limit

< 10-27 e-cm

< 10-29 e-cm

* M. Morse, private communication

1
2t N T

From beam line extension

From probing 545nm
transition with higher
Frank-Condon factor*

Improvement in Frank Condon Factor

FC factors
calculated from
RKR method
(R. Le Roy group)

* Dispersed Fluorescence data, courtesy of M. Morse group

Conclusion & Summary

Motivation

Methods

Search of Time symmetry violation

ground state of WC molecules

Measurements

Conclusion

Hyperfine

Sys. Uncertainty
of Eeff field

Identified 31 state of WC as

Doublet

Sys. Uncertainty
of g

WC Beam

Stat. Uncertainty

Analyzed systematic & statistical

uncertainties for eEDM expt.
with projected sensitivity of
|de| < 10-27 e-cm

candidate system for eEDM expt.

Thank You
Top Row: Jinhai Chen, Aaron Leanhardt, Emily Alden
Bottom Row: Kaitlin Moore, Yisa Rumala, Chris Lee, Erika Etnyre