Excited State: CaO, Cs, Rb Public
Bresler, Sean (Fall 2021)
Published
Abstract
Investigation of Rb, Cs, and CaO using gas phase spectroscopy will be described.
These molecules have been studied using the following techniques: laser-induced flu-
orescence (LIF), dispersed fluorescence, and laser induced photo-chemistry. Various
experiments were designed or modified including the folloing: flow cells, static cells,
vacuum chambers, and ion collection systems. Programs were written to control all
of these experiments and to produce the data reported.
Previous research suggests that diode pumped alkali lasers (DPAL) are a potential
route for high-powered laser design for use in ballistics defense and communication
due to their potentially favorable power scaling and useful wavelengths. Various
complications of these lasers are described, as well as attempts to quantify various
deleterious processes.
Laser induced fluorescence spectra for jet-cooled CaO have been used to examine the higher vibrational levels of the A′1Π(Xσπ–1) state (v = 10 - 17) and the v = 6-8 vibrational levels of the C1Σ+(Bσσ–1)state. A perturbation of v = 17 of the A’ state was evident, caused by a spin-orbit mediated interaction with the b3Σ+(Ω = 1)(Xσσ–1)v= 14 level. Ro-vibrational constants for the A’ state were obtained by fitting to the data for nominally unperturbed levels. The average radiative lifetime for the A′1Π(Xσπ–1) state v= 10–17 levels was10.6μs with no measurable dependence on v. This was consistent with the theoretical prediction of a relatively small transition dipole moment for the A′1Π– X1Σ+ band system. A homogeneous perturbation of the C1Σ+(Bσσ–1) v= 7 level was examined by means of dispersed laser induced fluorescence (DLIF) and radiative lifetime measurements.The DLIF spectra clearly demonstrate that the perturbing Ω = 0+ state is a component of a triplet state. Intense transitions from this state to the a 3Π(0+)(Xσπ–1)statewere observed. Configurational assignments are presented that support assignment of the perturbing state as the v = 12 vibrational level of the previously unobserved g3π(0+)(Bσπ–1) state.
Table of Contents
1 Product channels of Rb removal
1.1 Abstract.............
1.2 Introduction...........
1.3 Experimental ............................... 5
1.4 Results and discussion .......................... 7
1.5 Conclusions ................................ 16
1.6 Acknowledgements ............................ 17
2 Rb Removal By hydrocarbons 23
2.1 Rb*Removal ............................... 23
2.1.1 Summary ............................. 23
2.1.2 Background............................ 24
2.1.3 Experimental ........................... 26
2.1.4 Discussion ............................. 29
2.1.5 Funding .
3 Energy Pooling in Cs
............................ 34
35
..................... 1 ..................... 2
3.1 BackgroundandMotivation ....................... 35
3.1.1 Processes leading to higher excited states and ions of alkali vapor 36
3.1.2 Hydrocarbonbreakdownmechanisms . . . . . . . . . . . . . . 40
1
i
3.1.3 OpticalTrapping......................... 41
3.2 Experimentaldetails ........................... 42
3.2.1 ExperimentalConfiguration................... 42
3.2.2 LIFofCsH ............................ 43
3.2.3 Cesiumnumberdensitydetermination . . . . . . . . . . . . . 45
3.2.4 DLIF of Excited Cesium..................... 45
3.2.5 Pump-pump-probe cesium depletion experiment . . . . . . . . 46
3.2.6 Ion Collection Experiment.................... 46
3.2.7 Pooling and recombination.................... 48
3.3 Recommendations for future work.................... 50
4 Spin Orbit Mixing in Cs 57
4.1 Introduction................................ 57
4.2 Experimental ............................... 59
4.3 Results................................... 61
4.3.1 Kinetic Interpretation ...................... 61
4.3.2 Explanationof Stern-Volmer plots . . . . . . . . . . . . . . . 66
4.3.3 Noblegases,He,Ar,Kr ..................... 66
4.3.4 Methane, Ethane Results .................... 67
4.4 Discussion................................. 74
4.5 Conclusionsand Future Work ...................... 75
5 Perturbations of Calcium Oxide 76
5.1 Preface................................... 76
5.2 Introduction................................ 77
5.3 Experimental ............................... 80
5.4 Results................................... 82
5.4.1 LIFA-X.............................. 82
5.4.2 DLIF C-X . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 85
5.5 AnalysisandDiscussion ......................... 87
5.6 Acknowledgement............................. 93
5.7 SupportingInformation ......................... 93
A Appendix A: Linelists for CaO 94
B Appendix B: LIF System 103
B.1 SystemOverview ............................. 103
B.1.1 Ablation Translation/Rotation Holder . . . . . . . . . . . . . 103
B.1.2 Opticaltrain ........................... 106
B.1.3 Monochromator.......................... 106
B.2 Monochromator Source Code ...................... 107
B.2.1 Camera Attachment ....................... 124
Bibliography 126
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