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Atomic beam production and spectroscopy on the
    iron 3d64s2 5D4  3d64s4p 5D4 transition



   Bachelors presentation by Joost Jan van Barneveld



Facilities          Laser Centre Vrije Universiteit
Supervisors         Prof. Dr. Wim Ubachs
                    Dr. Eric-Jan van Duijn
Overview
•   Motivation – Why spectroscopy on Iron ?
•   Atomic beam production and setup
•   Theory of spectroscopy
•   Results
    – Resolving isotopes
• Discussion
    – Resolving hyperfine splitting
• Conclusion
• Debate
Introduction
                   • Shifting constant results in
                     renewed interest in spectroscopy1,2
                   • Iron is a suitable element:
                                – High universal abundance
                                – High mass number, Z=56
                                                 
                   •              Ehf   Z g (S I )        4      3




                                                                                                                                                  
Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
 [1] PRL 96, 151101 (2006) – W. Ubachs et al - Indication of a Cosmological Variation of the Proton-Electron Mass Ratio Based on Laboratory Measurement and Reanalysis of H2 Spectra
 [2] Nucl. Physics B 653 (2003) 256-278 - T. Dent, M. Fairbairn,
Beam production & setup
          • Elements need to be in gas phase for LIF
            spectroscopy
          • Evaporated iron forms a gas
          • Evaporation requires heat: 1808K




                                                                                Thermogravimetric Measurement of the
                                                                                Vapor Pressure of Iron from 1573 K to 1973 K
                                                                                Frank T. Ferguson, Joseph A. Nuth, and Natasha M. Johnson
                                                                                J. Chem. Eng. Data, 2004, 49 (3), 497-501 • DOI:
                                                                                10.1021/je034152w




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Beam production & setup
          1.    Fix the sample (iron curls)
          2.    Heat the sample
          3.    Contain the heat
          4.    Minimise speed distribution
                (Doppler width)




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Beam production & setup
          Fixing the sample
          • Sample holder needs to withstand the heat
          • Tantalum sheet (.5mm) is suited
          • Melting point 3269K




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Beam production & setup
          Heating the sample
          •     Hit the sample holder with inrared laser
                light (Nd:YAG 1064 nm)
          •     Sample absorbs the light and heats up
          •     Hot object emits blackbody radiation




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Beam production & setup
          Containing the heat
          •     Reflect IR radiation back to sample
          •     Minimize conduction




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Beam production & setup
          Assemble an oven
          • One vapour outlet
          • Keep the window clean




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Beam production & setup
          Reduce doppler broadening
          •     Parallel velocity broadens the spectral line
          •     Pick out atoms with perpendicular velocity
          •     Doppler width estimated 19 MHz


                                                                                            Excitation laser




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Beam production & setup
          Eventual setup
          • Frequency doubled tunable
            Ti:S laser
          • Atomic beam in vacuum:
            2.3*10-7 mBar
          • Observe fluorescence with
            PMT
          • Register wavelength with
            ATOS LM007




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Theory of spectroscopy
          Overview – Zooming in on quantum mechanics
          • Levels & Terms
          • Isotope shifts
          • Hyperfine splitting




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Theory of spectroscopy
          Levels & Terms
          • Quantum numbers
                – 3d64s2 5D4  3d64s4p 5D4
          • Aufbau principle
                – 2 electrons in every shell
                – Distribution amongst shells
                  determines Terms
                – Term symbols: 2s+1Lj
                – Iron has 5D4 in the ground state



Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Theory of spectroscopy
          Isotope Shifts
          • Normal, Specific and Field shift
          • Normal and specific shift
                – Kinetic terms due to wobbling of the
                  nucleus
                – Energy levels are influenced

                – Effect:  MS   Z  Z   (M NMS  M SMS )
                                           
                                   Z  Z 
                                                 me 
                                       M NMS 
                                                  mu



Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Theory of spectroscopy
          Hyperfine splitting
          • Caused by nuclear spin
          • Charge circling the nuclear B-field
            interacts as magnetic dipole
          • New quantum number:
                  
               F I J
          • Interaction energy:
                          A
                   E      F ( F  1)  J ( J  1)  I ( I  1)
                          2
                                                                                g s gi me
          • Splitting of levels                                    A  Z 3 4             mec 2
                                                                                  3 Mp

Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Summary
          • Evaporate iron to form a
            beam
          • Let the iron interact with the
            excitation laser
          • Quantum theory describes
            this interaction
          • Let’s analyse the
            measurements !



Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Results                                                                                     Fraction      Spin


                                                                                            54Fe   0.05845(35)   0

          Isotopes                                                                          56Fe

                                                                                            57Fe
                                                                                                   0.91754(36)
                                                                                                   0.02119(10)
                                                                                                                 0
                                                                                                                 ½
          •    Two isotopes easily                                                          58Fe   0.00282(4)    0
               found
          •    Intensity is directly
               proportional to isotope
               fraction
          •    Highest peaks
               correspond to highest
               fraction
          •    57Fe and 58Fe remain




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Results                                                                                     Fraction      Spin


                                                                                            54Fe   0.05845(35)   0
                                                                                            56Fe   0.91754(36)   0
          Isotopes                                                                          57Fe   0.02119(10)   ½

          •
                                                                                            58Fe
                57Fe   is split in four                                                            0.00282(4)    0

                 – Summed relative intensities
                   should relate to isotope fraction
          •     58Fe   is very weak
                 – Should have the same
                   distance from 56Fe as 54Fe




                       Z  Z 
               MS           ( M NMS  M SMS )
                       Z  Z 

Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Peak   Isotope   Position   Distance   Width

                                                                                 1      54Fe        -769        -       14.3
                                                                                 2      56Fe          0        769      14.3
                                                                                 3      57Fe        243        244      12.9
                                                                                 4      57Fe        455        212      18.2
                                                                                 5      57Fe        648        193      40.7
                                                                                 6      58Fe        735         86      32.1




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Discussion
          Hyperfine coupling constant

          •   E 
                     A
                       F ( F  1)  J ( J  1)  I ( I  1)
                     2
              EA  Ecg  2  ( A2  A1 )
              EB  Ecg  5 2 A2  2 A1
              EC  Ecg  5 2  A1  2 A2
                                                                                    Ecg
              ED  Ecg  5 2  ( A1  A2 )

                 2   2       1             EA 
                                 A1   E 
                 2 5 2      1       
                                    A2    B 
                5 2   2       1            EC 
                                 E   
                                         
                 5 2 5 2     1             ED 




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Discussion
                   Hyperfine coupling constant
                   • Which peak corresponds to                                                                                             Ecg

                     which transition ?
                             – Longest arrow highest
                               frequency
                             – Clebsch-Gordan coefficients
                   • Can we be sure that A1 and A2
                     are both positive ?
                             – A1 should be positive*
                                                                                       2   2            1         EA 
                                                                                                            A1   E 
                                                                                       2 5 2           1     
                                                                                                              A  B
                                                                                      5 2   2               2   EC 
                                                                                                          1 
                                                                                                           E   
                                                                                       5 2 5 2          1     
                                                                                                                     ED 


Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
 [*] Physical   Review V148 #1 1966 – “Hyperfine interactions and the magnetic fields due to core polarization in Fe”, W.J. Childs, L.S.
 Goodman
Discussion
                    Hyperfine coupling constant                                                                    Method            A1         A2        Ecg

                    • Options for matrix algebra                                                                   +,cgc              -24            24     511
                                                                                                                   +,-Ta                  43         47    445
                              – Omission of rows / least                                                           +,-Td                  47         43    447
                                squares                                                                            +,L. sq                45         45    455
                              – Clebsch gordan / Manual                                                            -, cgc             -24         -24       511
                                peak assignment                                                                    -, -Tb                 47         43    424
                              – Sign of second coupling                                                            -, -Tc                 43         47    424
                                constant                                                                           -, l. sq               45         45    428

                    • None gives the expected
                      result                                                                                                     2   2       1         EA 
                                                                                                                                                 A1   E 
                                                                                                                                 2 5 2      1     
                                                                                                                                                   A  B
                              – Values are in the order of                                                                      5 2   2          2   EC 
                                                                                                                                               1 
                                                                                                                                                E   
                                the literature values*                                                                           5 2 5 2     1     
                                                                                                                                                          ED 


Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
 [*] J.   Phys. B: At. Mol. Opt. Phys. 30 (1997) 5359–5365Optical isotope shifts in the iron atom - Bentony, Cochrane and Griffith
Conclusion
      • Fe Atomic beam production is possible
            – Oven can be improved to lengthen sample lifetime
      • Isotope splitting has been resolved
      • Hyperfine splitting has not been resolved
            – One more peak is needed to solve the system exactly
            – Excitation laser needs stability improvements




Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
Debate

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Atomic Spectroscopy of Iron Isotopes

  • 1. Atomic beam production and spectroscopy on the iron 3d64s2 5D4  3d64s4p 5D4 transition Bachelors presentation by Joost Jan van Barneveld Facilities Laser Centre Vrije Universiteit Supervisors Prof. Dr. Wim Ubachs Dr. Eric-Jan van Duijn
  • 2. Overview • Motivation – Why spectroscopy on Iron ? • Atomic beam production and setup • Theory of spectroscopy • Results – Resolving isotopes • Discussion – Resolving hyperfine splitting • Conclusion • Debate
  • 3. Introduction • Shifting constant results in renewed interest in spectroscopy1,2 • Iron is a suitable element: – High universal abundance – High mass number, Z=56   • Ehf   Z g (S I ) 4 3  Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion [1] PRL 96, 151101 (2006) – W. Ubachs et al - Indication of a Cosmological Variation of the Proton-Electron Mass Ratio Based on Laboratory Measurement and Reanalysis of H2 Spectra [2] Nucl. Physics B 653 (2003) 256-278 - T. Dent, M. Fairbairn,
  • 4. Beam production & setup • Elements need to be in gas phase for LIF spectroscopy • Evaporated iron forms a gas • Evaporation requires heat: 1808K Thermogravimetric Measurement of the Vapor Pressure of Iron from 1573 K to 1973 K Frank T. Ferguson, Joseph A. Nuth, and Natasha M. Johnson J. Chem. Eng. Data, 2004, 49 (3), 497-501 • DOI: 10.1021/je034152w Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 5. Beam production & setup 1. Fix the sample (iron curls) 2. Heat the sample 3. Contain the heat 4. Minimise speed distribution (Doppler width) Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 6. Beam production & setup Fixing the sample • Sample holder needs to withstand the heat • Tantalum sheet (.5mm) is suited • Melting point 3269K Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 7. Beam production & setup Heating the sample • Hit the sample holder with inrared laser light (Nd:YAG 1064 nm) • Sample absorbs the light and heats up • Hot object emits blackbody radiation Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 8. Beam production & setup Containing the heat • Reflect IR radiation back to sample • Minimize conduction Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 9. Beam production & setup Assemble an oven • One vapour outlet • Keep the window clean Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 10. Beam production & setup Reduce doppler broadening • Parallel velocity broadens the spectral line • Pick out atoms with perpendicular velocity • Doppler width estimated 19 MHz Excitation laser Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 11. Beam production & setup Eventual setup • Frequency doubled tunable Ti:S laser • Atomic beam in vacuum: 2.3*10-7 mBar • Observe fluorescence with PMT • Register wavelength with ATOS LM007 Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 12. Theory of spectroscopy Overview – Zooming in on quantum mechanics • Levels & Terms • Isotope shifts • Hyperfine splitting Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 13. Theory of spectroscopy Levels & Terms • Quantum numbers – 3d64s2 5D4  3d64s4p 5D4 • Aufbau principle – 2 electrons in every shell – Distribution amongst shells determines Terms – Term symbols: 2s+1Lj – Iron has 5D4 in the ground state Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 14. Theory of spectroscopy Isotope Shifts • Normal, Specific and Field shift • Normal and specific shift – Kinetic terms due to wobbling of the nucleus – Energy levels are influenced – Effect:  MS   Z  Z   (M NMS  M SMS )    Z  Z  me  M NMS  mu Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 15. Theory of spectroscopy Hyperfine splitting • Caused by nuclear spin • Charge circling the nuclear B-field interacts as magnetic dipole • New quantum number:    F I J • Interaction energy: A E  F ( F  1)  J ( J  1)  I ( I  1) 2 g s gi me • Splitting of levels A  Z 3 4 mec 2 3 Mp Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 16. Summary • Evaporate iron to form a beam • Let the iron interact with the excitation laser • Quantum theory describes this interaction • Let’s analyse the measurements ! Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 17. Results Fraction Spin 54Fe 0.05845(35) 0 Isotopes 56Fe 57Fe 0.91754(36) 0.02119(10) 0 ½ • Two isotopes easily 58Fe 0.00282(4) 0 found • Intensity is directly proportional to isotope fraction • Highest peaks correspond to highest fraction • 57Fe and 58Fe remain Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 18. Results Fraction Spin 54Fe 0.05845(35) 0 56Fe 0.91754(36) 0 Isotopes 57Fe 0.02119(10) ½ • 58Fe 57Fe is split in four 0.00282(4) 0 – Summed relative intensities should relate to isotope fraction • 58Fe is very weak – Should have the same distance from 56Fe as 54Fe  Z  Z   MS    ( M NMS  M SMS )  Z  Z  Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 19. Peak Isotope Position Distance Width 1 54Fe -769 - 14.3 2 56Fe 0 769 14.3 3 57Fe 243 244 12.9 4 57Fe 455 212 18.2 5 57Fe 648 193 40.7 6 58Fe 735 86 32.1 Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 20. Discussion Hyperfine coupling constant • E  A F ( F  1)  J ( J  1)  I ( I  1) 2 EA  Ecg  2  ( A2  A1 ) EB  Ecg  5 2 A2  2 A1 EC  Ecg  5 2  A1  2 A2 Ecg ED  Ecg  5 2  ( A1  A2 )  2 2 1  EA     A1   E   2 5 2 1     A2    B  5 2 2 1   EC     E      5 2 5 2 1  ED  Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion
  • 21. Discussion Hyperfine coupling constant • Which peak corresponds to Ecg which transition ? – Longest arrow highest frequency – Clebsch-Gordan coefficients • Can we be sure that A1 and A2 are both positive ? – A1 should be positive*  2 2 1  EA     A1   E   2 5 2 1    A  B 5 2 2   2   EC  1    E     5 2 5 2 1    ED  Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion [*] Physical Review V148 #1 1966 – “Hyperfine interactions and the magnetic fields due to core polarization in Fe”, W.J. Childs, L.S. Goodman
  • 22. Discussion Hyperfine coupling constant Method A1 A2 Ecg • Options for matrix algebra +,cgc -24 24 511 +,-Ta 43 47 445 – Omission of rows / least +,-Td 47 43 447 squares +,L. sq 45 45 455 – Clebsch gordan / Manual -, cgc -24 -24 511 peak assignment -, -Tb 47 43 424 – Sign of second coupling -, -Tc 43 47 424 constant -, l. sq 45 45 428 • None gives the expected result  2 2 1  EA     A1   E   2 5 2 1    A  B – Values are in the order of 5 2 2   2   EC  1    E    the literature values*  5 2 5 2 1    ED  Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion [*] J. Phys. B: At. Mol. Opt. Phys. 30 (1997) 5359–5365Optical isotope shifts in the iron atom - Bentony, Cochrane and Griffith
  • 23. Conclusion • Fe Atomic beam production is possible – Oven can be improved to lengthen sample lifetime • Isotope splitting has been resolved • Hyperfine splitting has not been resolved – One more peak is needed to solve the system exactly – Excitation laser needs stability improvements Introduction – Beam production – Spectroscopic Theory – Results – Discussion - Conclusion