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Atomic Physics Group Stockholm University Experimental Projects Instrumentation seminar November 28, 2002 Presented by Sven Mannervik Experimental work is primarily performed at the Manne Siegbahn Laboratory National Facility at Stockholm University G A,E: Laser spectroscopy D: Mass measurements B,G: Atomic collision F: Ion-electron recombination C: Ion- surface collision We use beams of highly charged ions from the electron beam ion source (EBIS) , the ECR ion source and stored ions in a synchrotron ion-cooler storage ring (CRYRING). With slow highly charged ions we study: • surface and cluster interactions • multiple electron transfer reactions • mass spectrometry of highly charged ions in a Penning trap In the ring we perform experiments with cooled stored ions •on electron-ion recombination and laser assisted excitation and recombination • on fast atomic collisions (single and multiple electron capture, ionization, recoil momentum spectroscopy) with internal target. •on laser spectroscopy, and lifetime measurements of metastable states at stored heavy ions. Lifetime measurements Why are radiative lifetimes needed? The radiative lifetime (t) is determined by the sum of the transition probabilities (Aik) for all decay channels t = S 1/ Aik Aik Excited state Metastable state Allowed transition A=108 s-1 Intensity I=NiAik Forbidden transition A=1 s-1 Why stored ion beam? 5 mm fast ion beam Laser 500 km ! •High spectral resolution (laser) •Time-resolution and long observation time A=108 s-1 A=1 s-1 •Pure light source (isotope separation) •Ultra high vacuum Instead of the passive method we use the active laser probing method E passive method M G PM Observation of spontaneous decay M G forbidden line Probing of the metastable population by laser excitation + higher efficiency + high selectivity + high flexibility PM Laser We gain a factor of 5000 and can reduce detector background. 100000 Intensity Laser probing technique (LPT) developed at CRYRING for lifetime measurements Ca_02_rp Lifetime: Ca+ 3d 2 D3/2 moving laser probe pulse 10000 1000 0 1 2 3 4 5 6 Time [s] Shutter synchronized with the ring creates laser pulses at variable time delays Laser probing technique – in summary Laser light Photon counts Higher level Lifetime curve Fluorescence Metastable level Lower level Moving probe pulse Time cycle 1 cycle 2 Photomulti plier CRYRING Laser cycle 3 Laser pulses Fluorescence yield Time after injection Number of injected ions has to be constant! The FERRUM project Photon counts 10000 62 metastable levels 4 1000 b D7/2 100 a 6S5/2 10 1 0 1000 2000 Time [ms] Laser probing of a 6S 5/2 z6D7/2 6516 Å a6S5/2 a6DJ 1/2 3/2 5/2 7/2 9/2 Eta Carinae blob 3000 Results Fe II Level Quinet et al SST 262 ms Experiment a6S5/2 Garstang Nussbaumer Quinet et al et al HFR 326 ms 235 ms 220 ms b4D7/2 618 ms 500 ms 567 ms 530(30) ms a4G9/2 856 ms 694 ms 755 ms 650(20) ms 5.20 s 6.59 s 3.8(0.3) s b2H11/2 10.1 s 230(30) ms Rostohar et al Phys Rev Lett 86(2001)1466 Experimental results Ti II 2 c D3/2 base pressure 2000 c 2D3/2 : 0.35 0.05 s 34 metastable levels 1000 0 0 0,5 1 1,5 Time [s] c 2D3/2 b4 P5/2 base pressure Long lifetime – very sensistive to corrections 1000 b 4P5/2 100 10 0 10 20 30 40 Tim e [s] Preliminary 27 10 s 50 Ground level a 4F3/2 Ion beam Collinear geometry gives subDoppler line width Laser beam Laser and Radio-Frequency double Fluorescence Intensity [counts] 4000 F=9/2 F=7/2 3000 Dn=200 MHz F=5/2 2000 151Eu+ =5818 Å F=1/2 F=3/2 1000 0 resonance spectroscopy 0 2 Observed Peak 1 Peak 2 Generated Curve 2100 2000 Dn<1 MHz Counts 1900 1800 1700 1600 1500 795085 795585 796085 796585 797085 Frequency [kHz] 797585 798085 4 Relative Frequency [GHz] 6 8 Ion-electron interaction cooling SBD Electron Cooler recombination Dipole Magnet e Aq Aq 1) hn Recombination Overview Radiative Recombination is an direct spontaneous process in which a continuum electron is captured with the subsequent release of a photon e Aq Aq 1)** Aq 1)* hn Dielectronic Recombination is a resonant process in which a continuum electron is captured as it excites a target electron, forming a short lived intermediate state which decays by photon emission Experiment CRYRING 2 2 mv2 mv|| D ) m m f v ) = exp 2k BT 2k BT|| 2 k T 2 k T B B || 1 SBD Electron Cooler Dipole Magnet Used for radiative recombination studies of ions with free electrons at CRYRING10 14+ Si Si14+ 4 B Laser induced recombination into specific quantum states enhancement factor 200 = 90o o = 45 o = 0 = -45o o 15 V/cm - 0 o 15 V/cm - 45 o 15 V/cm - 90 200 p+e- H(n=3) Gain 150 50 0 0 10 Relative Energy (meV) 103 N7+ He++ 102 He2+ 101 D+ 100 10-1 0 10-6 10-6 10-4 10-5 20 10-4 10-3 10-2 10-1 10-2 100 Energy Relative Energy (eV) E 100 -10 Rate Coefficient (10-12 cm3/s) Influence of external (electromagnetic) fields on recombination rate Si14+ E 100 (eV) Laser Ring with an Implemented Amplifier AC FS2 FS1 Nd:YAG Laser 2nd harmonic PC WP HVP PD1 PD2 Excimerdye laser The optical laser ring with the implemented amplifier gives a total gain of about 23 in comparison with a single passage of the pulse through the interaction zone. SBD Electron Cooler Dipole Magnet T. Mohamed, G. Andler, R. Schuch, subm. to J. Opt. Com. Dielectronic recombination (DR) process C3+ +e ‘allowed’ process C2+ 1s22sg 3Ge e- 1s22p4f 3Ge Coulomb interaction ‘forbidden’ process 1s22p4d 3Do 1s22sf 1Fo 4d 1Po Spin-orbit 4d 1Fo 4f 1De interaction 4p 1Se 4f 1Ge 0,25 1 e 4f F Energy [eV] a . First ionization limit 4p 1De 4d 1Do -0,25 3 0 0 4f 3De 4d 3Do 4d 3Po 4p 3Se 4p 1Pe 3 -0,75 4s 1Po -1,25 4f 3Ge Ionization 1 limit 0 0 4f 3Fe 3 e 4d 3stabilization Fo 4pRadiative P 4p D 1s22p2 3P DRrate[10 -12 cm 3/s] DRrate[10 -12 cm 3/s] e-0,75 5 0 0 e 4 0 b . 1 5 0 0 1 0 0 6 0 3 0 0 2 1s 2p3d 3Fo 2 0 0 . 2 0 . 4 0 . 6 1 0 0 4s 3Po 0 . 1 0 . 3 0 . 5 E n e r g y [ e V ] 0 . 7 Experiment 350 (a) 300 Counts 250 200 150 100 50 0 (b) Lab Energy [eV] 5000 4800 4600 4400 4200 CM Energy [eV] 4000 (c) 6 4 2 0 0 1000 2000 3000 Channel 4000 5000 6000 Importance of knowing the ring length Relative position •S6 •Beam profile monitor •Two cooler scrapers Dv = f f Absolute length •Laser induced recombination •Measurement of the difference between DR resonances 1 0 )L Li-like Kr Madzunkov et al., Phys. Rev. A65, 032505 (2002) QED effects are small for high-n, so these states can be calculated accurately 2p1/2 2s Rate Coefficient x 10 -9 [cm3 s-1] 15 l 12 71.243(8) Exp. Uncertainty Exp. 71.248(19) 10 Theory Uncertainty QED 8 6 4 2 0 4.0 4.2 4.4 4.6 4.8 5.0 5.2 5.4 5.6 Energy [eV] Energy Splitting E2 s1 2 2 p1 2 = Enl We are now doing… “Quantum electrodynamics in the dark” Physics World, Aug. 2001 Ni17+ + e Ni16+ Fast ion-atom collisions Transfer Ionization in MeV p-He Collisions Studied by Pulsed Recoil-Ion-Momentum Spectroscopy in a Storage Ring/Gas Target Experiment p-HeH0+He2++e- at 2.5-4.5 MeV Fast Ion-Atom collisions in CRYRING CRYRING: High Current (100 A H+) Cold and narrow beam ( 1 mm) The Gas-Jet Target: Density: up to 1011 cm-3 Jet diameter: 1.0 mm Luminosity: 61024 cm-2s-1. TI-rate @ 4.5 MeV: 1 min-1. SI-rate @ 4.5 MeV: 107 s-1. PROJECTILE DETECTOR GAS TARGET Gas jet Transfer Ionization in fast H+-He collisions: Thomas p-e-e scattering He p v 45 2v 0.55 mrad o v v pR0 The He nucleus is not directly involved in the collision RIMS! Kinematical Transfer Ionization (KTI) Kinematical capture through momentum overlap. p e- v v He Shake-off H He2+ pR-Q/vp-mevp/2 The He nucleus is emitted in the backward direction as a result of the pR=5.0 au @ 2.5 MeV kinematical capture. (ER~50 meV) The pulsed spectrometer: Recoil detector images. KTI/(SC+TI) 5 4 2+ He /(He +He ) [%] Total TI KTI 2+ + 3 2 Shake-off limit: 1.63% ??? 1 0 0 5 10 v(v0) 15 20 Highly charged ions produced in CRYSIS an EBIS Slow Highly Charged Ions Colliding with C60 – stability and fragmentation q+ e- e- e- Aq+ Collimated C60 Jet T=500 C Vex Experimental set-up Time-of-flight 0 V -100 V Cylindrical analyzer TRIG (q-s)+ START PSD STOP q+ A Multi-hit TDC 4+ C605+ C60 C60 C60 C607+ 6+ PSD 29+ C603+ 28+ 27+ Xe30+ + C60 Xe28 ++ …. Time-of-flight 26 keV Ar8+ + C60 Ar(8-s)+ + ... Counts 100 4+ s = 1 3+ C60 250 2+ C60 200 4+ C60 50 + C60 Cold 0 2000 3000 4000 5000 6000 7000 Counts 150 s = 3 8000 Counts 100 0 60 40 20 0 6+ C60 + C3 C60 3+ + C60 C4 3000 3000 + C5 4000 time-of-flight (channel number) 5000 C3 + C4 4000 + 5000 6000 C6 s = 4 + C7 + C9 + C8 10 0 2000 2000 + 4+ 2+ C60 C60 30 20 80 3+ C60 C60-2m time-of-flight (channel number) C60 7+ 5+ C60 6+ 50 5+ C60 3+ 100 Counts 120 4+ C60-2m 150 time-of-flight (channel number) 140 s = 2 C60 2000 + + C10 C11 Hot + C12 3000 time-of-flight (channel number) 4000 Decay channels of excited C60: Evaporation of small neutral fragments (C60r+)* C60-2mr+ + C2m (m=1,2,3,4…) Activation energy Ea for evaporation of a C2 unit ~10 eV dominate for r 3 Asymmetric fission r+ (C60 )* C60-2m(r-1)+ + C2m+ U(R) (m=1,2,3,4…) dominate for r 4 Decay rate: k 1/exp( Bfis / kBT) Depends on internal energy or temperature of C60 decrease T increase lifetime Bfis C60r+ Ekin C58(r-1)+ + C2+ R kinetic energy releases fission barriers Multifragmentation: stability (C60r+ )* many small fragments in low charge states Storage and lifetime measurements of C60 ions using ConeTrap: An Electrostatic Ion Trap for Atomic and Molecular Physics -electrostatic -simple -small -easy to cool 8 mm 175 mm H.T. Schmidt, H. Cederquist, J. Jensen, and A. Fardi, NIMB 173, 523 (2001). Mass determinations with highly charged ions relevant for fundamental physics Ions from CRYSIS SMILE Trap How to measure atomic mass with very high precision? n- 810 Hz n+ 36 MHz nz 240 kHz • Principle : Measurement of the cyclotron frequency of an ion trapped in a homogeneous magnetic field : 1 qeB nc = 2 m Dm Dn c = m nc using HCI the precision increases linearly Frequency Detection • nc is scanned and the ion TOF is measured • A resonance is detected : R ESO N A N C E SPEC TR U M FO R 76 Se 25+ 1s excitation / 15 hours 85 80 Relative uncertainty = 0.57 ppb Tim e-of-flight (µs) 75 1.0000 ± 0.0399 H z 70 1.0 Dn c [Hz] Texc [s] 65 60 55 23 852 936.0726 ± 0.0135 H z 50 34.5 35.0 35.5 36.0 36.5 37.0 37.5 38.0 23 852 9XX.XX [Hz] • To avoid the B dependence the unknown mass is deduced from the ratio: R= • nc n cREF qmREF = qREF m the reference ion is 12Cq+ or H2+ The atomic mass m is obtained by correcting for the missing q electrons and binding energies Where does the mass of an atom or ion matter • 28Si • 76Ge for Atomically Defined Kilogram Mass Standard an 76Se gives the Q value for the neutrino-less double beta decay • 133Cs, • 24Mg • 198-204Hg • binding energies from Aq+, Aq-1, Aq-2 ... for Accurate Determinations of the Fine Structure Constant and 26Mg for bound-electron g factor determination in hydrogen-like ions to solve the “mercury problem” in Audi/Wapstras mass table … a relative mass accuracy of dm/m = 10-9-10-10 is required Highly Charged Ions on Surfaces ECR – a new ion source medium high charge state on high voltage platform Pb55+ on Ta: Rc72 a.u. nc 53 Filling and cascading mechanism ? How fast charge-state equilibrium reached? Time until hollow atom is relaxed ? Auger transitions X-ray transitions 8.5 q keV Pb55+: t6 fs Side-feeding -Below surface relaxation ? Auger and X-ray spectroscopy, transmission exp -Above surface relaxation ? Grazing Angle Scattering Large angle Scattering Arq+ Au(111) Neutralization Charge State Distribution Energy loss X-ray Measurement Pbq+ Ta Absorption Method Below surface relaxation Ion beam Left Si(Li) detector dFront dBack Ta foil Moveable Faraday cup Pb53+ Foil thickness determined by Rutherford backscattering technique Right Si(Li) detector 8.5 q keV Mean Emission Depth 44 nm (about 100 monolayers) 0,0018 Intensity [per incident ion] Focusing system Front-spectra Back-spectra 0,0016 0,0014 0,0012 0,0010 0,0008 0,0006 0,0004 0,0002 2,5 3,0 3,5 Energy [eV] 4,0 4,5