Institut für Physikalische Chemie & Elektrochemie, Lehrgebiet A Columbus, OH, June 2006.ppt Zentrum...

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Columbus, OH, June 2006 <Dateiname>.ppt

Zentrum für Festkörperchemie

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Columbus, June 2013

ROTATIONAL SPECTRAIN SERVICE OF PARTICLE PHYSICS

- ZEEMAN & HYPERFINE EFFECTS

Jens-Uwe Grabow, Lukas D. AlpheiGottfried-Wilhelm-Leibniz-Universität Hannover

Richard J Mawhorter, Alexander Baum, Zachary Glassmann, Benjamin GirodasPomona College, Claremont, CA

Trevor J SearsBrookhaven National Laboratory, Upton, NY

N.E. Shafer-RayUniversity of Oklahoma, Norman, OK

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Advantages of FT-microwave spectroscopy

Sample preparation for FT-MW Experiment

Precise FTMW Characterization

Future High Precision FTMW Investigation

Rotational Spectroscopy in the Time-Domain:Technique, Capabilities & Directions

non-volatile species: LASER-Ablation Source: CATS technique

high resolution & sensitivity: Resonator & Jet: COBRA instrument

electronic angular momentum species: in-situ generation: PbF, YbF, etc.

- Stark effect

- Zeeman effect

e-EDM sensitive species: Polarization direction: DREAM-FTMW machine

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Coaxial oriented Beam-Resonator Arrangement (COBRA):molecular excitation

)()(

)()(

tt

tt

bbba

abaa

0 baab

tMW pulse

1μs

before excitation pulse: dipole moments cancelEb

Ea

many two-level systems

single particle, Schrödinger equation:

iH

iH ,ensemble properties, von Neumann equation

wavefunction

density matrix

density matrix:

(no) coherence:

population: 0 bbaa

J.-U. Grabow, W. Stahl, Z. Naturforsch. 45a, 1043 (1990).

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Coaxial oriented Beam-Resonator Arrangement (COBRA):molecular response

E

t

T = 100μs

MW signal

after excitation pulse: oscillating macroscopic dipole moment

density matrix:

)()(

)()(

tt

tt

bbba

abaa

0, baabcoherence:

population: 0bbaa

Fourier Transform

Frequency Domain, Spectrum

Time Domain, FID

U. Andresen, H. Dreizler, J.-U. Grabow, W. Stahl, Rev.Sci.Instrum. 61, 3694 (1990).

J.-U. Grabow, W. Stahl, H. Dreizler, Rev.Sci.Instrum. 67, 4072 (1996).

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COBRA chamber

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Fabry-Pérot Type Resonator: Spherical Reflectors

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Spherical Reflector: Transmit & Receive Antennae

supersonic-jet source

high-frequency antennae

low-frequency antennae

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TeSe: Electronic Data From Pure Rotational Spectra

125Te77SeJ‘ ← J 4 ← 3

Resolution:0.0000001 cm-1

Accuracy:0.00000001 cm-1

req = 235.904038(71) pm

Deike Banser, Melanie Schnell, Jens-Uwe Grabow, Emilio J. Cocinero, Alberto Lesarri, and Jose L. Alonso, Angew. Chem. Int. Ed. 2005, 44, 6311.

3

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MSe Multi-Isotopolog Potential Fits:Tracking down tiny effects of different origin

, ,

L. Bizzocchi, B.M. Giuliano, M. Hess, J.-U. Grabow, J. Chem. Phys. 126, 114305(2007).

B.M. Giuliano, L. Bizzocchi, S. Cooke, D. Banser, M. Hess, J. Fritzsche, J.-U. Grabow, PCCP 10, 2078(2008).

Born-Oppenheimer breakdown correction coefficients:

)24(92.12)(01 PbSePb

)16(915.1)(01 PbSeSe

)19(644.1)(01 SnSeSn

)10(841.1)(01 SnSeSe

)71(9787.20)(01 TeSeTe

)32(9541.20)(01 TeSeSe

1 3 1electronic state nuclear volume

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Symmetry leads to ±M-degeneracy of any molecule/atom that is not broken by an E-field along quantization axis.

The existence of an electron electric dipole moment would break this symmetry.

Major Difficulty:

A backgroundmagnetic field mimics an electron EDM.

What Would An

electron Electric Dipole Moment (e-EDM)

Do?

To search for an e-EDM look for

DU=U+M –U-M

in a strong (internal) E field at alternately parallel/anti-parallel B-fields.

A polar heavy atom diatomic in an electric field parallel or anti-parallel to an magnetic field:

• with a zero e−EDM the energy between states that differ only by MF is independent of the relative direction.

• a nonzero e−EDM would cause a small difference in this energy for the parallel and anti-parallel

configuration.

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Molecules with electronic angular momentum:

Heavy-metal fluorides

PbF

un-paired p electron: 2P1/2 ground state small g-factor

hfs due to F (and 207Pb) spin I = 1/2 large polarizabilityheavy Pb nucleus: relativistic effects candidate for e-EDM measurements @ reasonabe B-field control

\w linear Stark-effect (Eint~30 GV/cm) at moderate ext. fields

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Generation of PbF seeded supersonic jet:Coaxial Ablation Twin Source (CATS)

SF6(1%) / Ne @ ~500 kPa

Nd:YAG LASER I

Nd:YAG LASER II

supersonic

expansion

rotating/translating rods: elements, alloys, compounds

bulk material, compressed powder

elementary Pb

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Zeeman-effect of 208PbF

-0.6 -0.4 -0.2 0 0.2 0.4 0.6 0.8

-0.15

-0.1

-0.05

0

0.05

0.1

0.15

0.2

Parallel ...

Splitting/MHz

B / gauss

Perpendicular Magnetic Field: ∆M = ± 1

Parallel Magnetic Field: ∆M = 0J, F = 1/2, 0 → 3/2, 1

J, F = 1/2, 1 → 3/2, 1

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Molecules with electronic angular momentum /w nuclear hfs:

Concept for a molecular spectroscopy e-EDM experiment

accidentally close-lying 207Pb19F states of opposite parity: complete polarizability (yielding ~30GV/cm effective internal fields) at moderate laboratory E fields (200V/cm)

2-spin system:

e-, F

3-spin system: e-, F, Pb

208Pb19F 207Pb19F

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Molecules with electronic angular momentum w/o nuclear hfs:

Concept for a molecular spectroscopy e-EDM experiment

WC:3Δ1electronic ground state

small g-factor

Systematically very

close-lying Λ-doublets

of opposite parity:

fields of E ~ 1 V/cm are

sufficient for complete

polarization (60 GV/cm).

from A. Leanhardt

Current limit (de =10.5 x 10-28 e cm-1):

would lead to e-EDM effect of 50 mHz

E = 0 E ≠ 0

J = 2

J = 1

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Where are we now?

accuracy reached with:

- standard COBRA-FTMW instrument

- <5 d after Pb rod was first inserted

measurement linewidth comparable to that in study of YbF:

J. Hudson, B. Sauer, M. Tarbutt, E. Hinds, Phys. Rev. Lett. 89 (2002) 23003.

Ai = -di + dci J(J+1)alternative interpretation of dci:

centrifugal correction to Ai

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Origin Of dc1 And dc2 ?Comparison to high level ab-initio calculations

in preparation

FS-RCCSD method

large basis sets

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Where are we now?

nuclear anapole moment

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PbF: P-odd, T-odd effects

Current limit (from Tl atomic spectroscopy): de =10.5 x 10-28 e cm-1

J. J. Hudson, D. M. Kara, I. J. Smallman, B. E. Sauer, M. A. Tarbutt, E. A. Hinds, Nature 473 (2011) 493

corresponds to: WP,T κP,T+ Wd de = 17 mHz

nuclear anapole moment constants e-EDMV. V. Flambaum, I. B. Khriplovich, O. P. Sushkov, Phys. Lett. B 146 (1984) 367.

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P-odd – Interaction Constant Wp:ab-initio calculations

A. Borschevsky, M. Ilias, V. A. Dzuba, K. Beloy, V. V. Flambaum, P. Schwerdtfeger, Phys. Rev. A 85, 052509 (2012)

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Ytterbium Fluoride

YbF

un-paired s electron: 2S1/2 ground state small g-factor

hfs due to F spin I = ½ (171/173Yb: 1/2,5/2) large polarizabilityheavy Yb nucleus: relativistic effects

candidate for e-EDM measurements @ precise B-field controls electron penetrates nucleus: nuclear anapole moment sensitivity

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Generation of WC seeded supersonic jet:Coaxial Ablation Twin Source (CATS)

SF6(1%) / Ne @ ~500 kPa

or

pure Ne @ ~500 kPa

Nd:YAG LASER I

Nd:YAG LASER II

supersonic

expansion

rotating/translating rods: elements, alloys, compounds

bulk material, compressed powder

elementary Yb

or

YbF

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COBRA-FTMW YbF Measurements

Measured 12 new and 4

previous* YbF lines:

• 1 170YbF lines

• 4 171YbF lines#

• 4 172YbF lines

• 4 174YbF lines

• 3 176YbF lines

# Spin ½ Yb nucleus

174YbF

*C.S. Dickinson, S.A. Coxon, N.R. Walker, M.C.L. Gerry , J. Chem. Phys. 115, 6979 (2001).

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YbF multi-isotopologue fit#+ results

174Yb19F V=0 V=1

Y01 / MHz 7256.444(80)

01 / MHz -0.145(80)

Y11 / MHz -44.9378(152)

Y02 / MHz -0.007159* -0.006904*

/ MHz -13.418163(310) -33.80950( 49)

D / MHz 0.00397552(309) 0.0043202( 37)

bF(F) / MHz 170.26361( 68) 168.8030(110)

c(F) / MHz 85.4035( 32) 86.7127(134)

cD(F) / MHz 0.001552( 70) 0.00216( 38)

CI(F) / MHz 0.014544(177) 0.01548( 66)* fixed to value taken from:

K.L. Dunfield, C. Linton, T.E. Clarke, J. McBride, A.G. Adam, J.R.D. Peers, J. Mol. Spectrosc. 174, 433 (1995).

+ including RF transitions taken from:

B. E. Sauer, J. Wang, and E. A. Hinds, J. Chem. Phys. 105, 7412 (1996).

# including v=1 transitions taken from:

C.S. Dickinson, S.A. Coxon, N.R. Walker, M.C.L. Gerry , J. Chem. Phys. 115, 6979 (2001).

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Diatomic Rotation - The quest for thee-EDM accelarated by Molecular Spectroscopy:

DREAM - FTMW

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Acknowledgement

Aaron Leanhardt, U. Michigan

Feinmechanikwerkstatt des Instituts für Physikalische Chemie

W. Rogge

Deutsche

Forschungsgemeinschaft (DFG)

Deutscher Akademischer

Austauschdienst (DAAD)

Fonds der Chemischen Industrie

(FCI)

Land Niedersachsen

Institut für Physikalische Chemie & Elektrochemie, Lehrgebiet A Columbus, OH, June 2006.ppt Zentrum...

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Transcript of Institut für Physikalische Chemie & Elektrochemie, Lehrgebiet A Columbus, OH, June 2006.ppt Zentrum...