Laser Spectroscopy of HeH + 施宙聰 2011 AMO TALK 2011/9/26
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1 Laser Spectroscopy of HeH + 施宙聰 2011 AMO TALK 2011/9/26
2 Outline Introduction Previous experimental results Saturation spectroscopy Conclusions and future works
3 Diatomic Molecules Total energy=electronic energy + vibrational energy + rotational energy E tot = E elec + E vib + E rot E elec ~ few ev E vib ~ E elec /100 E rot ~ E vib /100 Rovibronic transition Vis, UV Rotation-vibrational IR Rotational mwave, THz
4 Simple Diatomic Molecules One-electron: H 2+, HD +, D + 2 Two-electron: H 2, HD, D 2, HeH + HD +, HeH + : electric dipole moment for rotation-vibration transitions
5 Why HeH +? One of the simplest two-electron diatomic molecules: benchmark of theoretical calculation It is formed by hydrogen and helium, the two most abundant elements in the universe. It is the first molecule in the universe. HeH + had been suggested presenting in the astronomical objects such as nebula, super nova, white dwarfs and quasi-stellar object (QSO)envelop.
6 Potential curves of HeH + Ground electronic level H.H. Michels, J. Chem. Phys., 44, 3834 (1966).
7 Theoretical calculations Born-Oppenheimer (BO) approximation Non-adiabatic calculation Relativistic corrections QED corrections
8 Generation and destruction of HeH + Generation He * +H 2 HeH + +H+e H 2+ (v 3)+He HeH + +H Destruction HeH + +H 2 He +H + 3
9 Spectroscopic methods Doppler-tuned ion beam spectroscopy Laser absorption spectroscopy in discharge
10 Spectroscopy Using Ion Beam Willis Lamb ( ) 1955 Nobel prize Mossbauer effect Lamb shift Laser physics Lamb dip William H. Wing University of Arizona
11 Doppler tuning: tuning range depends on laser frequency, ion mass and accelerating voltage High resolution: velocity compression Linewidth ~ 10 MHz Collision detection: low signal-to-noise ratio
12 Spectroscopy Using Discharge Gerhard Herzberg ( ) 1971 Nobel prize in chemistry Takashi Oka First observation of H 3 + IR spectrum
13 Observation of H + 3 IR spectrum by Oka (1980) Tunable DFG source LN2 cooled hydrogen discharge Absorption spectrum with 32 m length Observation of HeH + fundamental band spectrum by Bernath and Amano (1982) 4% absorption for R(1) transition in fundamental band
14 Velocity Modulation Spectroscopy Sensitive to ions not to neutrals Richard Saykally (UC Berkeley) 1983
15 Taken from Prof. B.J. McCall s talk
16 Taken from Prof. B.J. McCall s talk
17 Taken from Prof. B.J. McCall s talk
18 Laser Spectroscopy of 4 HeH + Authors Method Measured Transitions [1979] D.E. Tolliver, G. A. Kyrala and W.H. Wing Ion beam Fundamental Band : P(12)-P(13) ν = 2-1 : P(9)-P(11) Accuracy (MHz) 60 [1982] P. Bernath and T. Amano Absorption Fundamental Band : R(0)-R(4) and P(1)-P(4) 30~60 [1989] M.W. Crofton, R.S. Altman, N.N. Haese and T. Oka VM ν=1-2 R(1)-R(5), R(8), P(1) and its isotopes 60 [1997] F. Matsushima, T. Oka and K. Takagi VM Low J pure rotation R(0) and R(1) [1997] Z. Liu and P.B. Davies VM Quasi-bound to quasi-bond and bond to quasi-bond
19 HeH + Pure Rotation Transitions Tunable FIR source: two CO 2 lasers + microwave + MIM diode frequency up to 6 THz mw power LHe cooled bolometer Oka and Takaji 1997 The lowest J = 1 0 transition of 4 HeH + observed at (2) GHz will be an important future probe for detecting this species in space.
20 Saturation Spectroscopy of Molecular Ions (H 3 + and HeH + )
21 How to achieve? > Light Source CW Optical Parametric Oscillator ---- Enough power for saturation. > Extended Negative Glow Discharge Tube ---- Low pressure, high concentration of ion. > Optical Frequency Comb ---- Frequency ruler for precision measurement.
22 PPLN (periodically poled LiNbO 3 ) Quasi-phase matching High nonlinear efficiency over 0.4 to 5 mm Taken from HC Photonics
23 Singly Resonant PPLN OPO Unlike other MIR light source, OPO provides larger power which is benefit for the saturation spectroscopy of molecular ion. Idler Wavelength: μm Average Power: > 300 mw Frequency Tuning: > 40 GHz (Mode-Hop-Free) Free-Running Stability: < hours Pump: 1062 nm alpha-dfb laser boosted to 6 W by a YDFA
24 Glow Discharge Features of negative glow region: n + Largest glow intensity Highest concentration of positive ions Nearly field free The region is relatively short n -
25 Extended Negative Glow Discharge Negative glow Region - B field (> 300 Gauss) + Benefits of extended negative glow : Lower gas pressure (~100 mtorr) Narrower linewidth for precision measurement Flow mixture of He:H 2 = 98 : 2 (120 mtorr) Discharge Current : 16 ma Ethanol cooled at -70 o C Discahrge length = 150 cm
26 Experimental Setup for saturation spectroscopy Pump Power: ~110 mw Beam Size: 1.75 mm (Diameter, 1/e 2 ) Probe beam ~ 10 mw The intensity is ~ 40 kw/m 2
27 Absorption Doppler Broadened Spectrum HeH + R 0 (1) at GHz 1.5x x MHZ (~ 200 K) 5.0x x Frequency Tuning (MHz)
28 Amplitude 3 rd Derivative Spectrum HeH + R(1) Transition S/N ~ 100 msec Frequency Tuning (MHz) Frequency Modulation Method (by modulating the pump frequency) Modulation Frequency : 31 khz Modulation Depth : 7.6 MHz Laser Intensity : ~ 40 kw/m 2 (or 40 mw/mm 2 )
29 Amplitude (A.U.) Linewidth analysis 4 HeH+ R 0 (1) Linewidth Investigation of Sub-Doppler Feature 2.5x x x x10-3 Linewidth: 6.6 +/- 0.2 MHz 5.0x Modulation Depth (MHz) - Peak to Peak Fitting Function : HM Fang et. al., Opt. Comm., 257, 1, (2006)
30 ITRI Fiber OFC Repetition Rate : 250 MHz Supercontiuum : 1030 ~ 2200 nm RF Reference : GPS-locked Rubidium clock Accuracy : < 1000 sec (~few khz in the MIR region) μm μm μm
31 Frequency measurement
32 Frequency Deviation (MHz) Frequency measurement results HeH + R0 (1) Absolute Frequency Measurement MHz Counts
33 Conclusions and Future Works First observation of saturation spectrum of HeH + Absolute frequency measurement better than 100 khz (~1 ppb accuracy) In future Saturation spectroscopy of H 3+, HeD + Velocity modulation spectrum of HeH + and HeD + using PPLN DFG (breakdown of BO approximation)
34 Acknowledgements We thank to the National Science Council (NSC), Ministry of Education, Natural Science and Engineering Research Council of Canada ( NSERC ) and Industrial Technology Research Institute.
35 Thanks For your Attention!
36 Frequency Comb Ti:Saphire Kerr-lens mode locked laser w r =1/T, T: repetition time Controlled by cavity length D pulse-to-pulse carrier envelope phase shift Controlled by pulsed power 2007/12/07 36
37 f-2f self-reference Dn/n = 1X 上限 Dn/n = 1X /12/07 37
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