VUV Spectroscopy of Atoms, Molecules and Surfaces

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146 REFERENCES [62] S. Baier et al., J.Phys.B27, 1341 (1994). [63] M. Gisselbrecht et al., J.Phys.B31, L977 (1998). [64] P. Erman et al., Chem. Phys. Lett. 239, 6 (1995).
Summary For an atom or molecule in the gas phase or at a solid surface, the spatial distributions of the electrons with respect to the nucleus and of the nuclei with respect to each other are reflected in the electronic-, vibrational- and rotational energies of the system. By the quantum-mechanical rules governing such a system, only certain (discrete) energies, so-called stationary states, are allowed, and the elucidation of these states and their stabilities, or lifetimes, is at the heart of atomic- and molecular spectroscopy. According to the Heisenberg uncertainty relation, the decay of a stationary excited state is associated with a broadening of the corresponding energy level. As a consequence, the stability of the state can be determined from a measurement of either the lifetime or the spectral width of the energy level. Following an external, non-perturbative disturbance by, e.g., a light field, the nuclei of the atoms bound in a molecule or a solid may undergo a spatial re-arrangement, as reflected by a dynamical change in the energy-level diagram. A structural dynamical transition involves the breaking (and possible formation) of intra- or inter-molecular chemical bonds and proceeds on the atomic level on a femtosecond (10 −15 s) time scale. Examples of such transitions are the dissociation of a molecule following its excitation to a repulsive state, a chemical reaction or a solid-liquid phase transition. The present thesis is concerned with the spectroscopic investigations of electronically excited, stationary states of gas-phase atoms and -molecules, in particular negative ions, and of structural dynamical transitions of molecules bound to solid surfaces. A common element of most of these studies is the use of laser light in the vacuum-ultraviolet (VUV) part of the electromagnetic spectrum, i.e. the 10–200 nm wavelength range. The generation of light with a narrow spectral bandwidth or a femtosecond pulse duration, as required for the studies of the thesis, is not as straightforward in the VUV as in the visible regime. An overview of the present status of VUV light generation with emphasis on the present spectroscopic possibilities and limitations imposed by the quality of the light source is the subject of chapter 1.
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VUV Spectroscopy of Atoms, Molecule
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ii CONTENTS 4 .6 Conclusion . . . .
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iv Experimental and theoretical stu
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vi me to the principle of negative-
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viii
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2 VUV light generation: possibiliti
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10 VUV light generation: possibilit
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18 REFERENCES [14 ] C. R. Vidal, in
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20 REFERENCES [55] C. J. G. Uiterwa
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22 REFERENCES [98] Parameters from
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24 Negative ions ing the binding en
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26 Negative ions located energetica
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28 Negative ions available has been
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30 Negative ions assignment will th
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32 Negative ions feel the repulsion
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34 Negative ions Figure 2.1: Adiaba
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36 Negative ions
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38 REFERENCES [16] E. Kopp, Adv. Sp
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40 REFERENCES [63] P. Balling et al
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42 REFERENCES
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44 High-resolution VUV spectroscopy
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60 REFERENCES [19] J. S. Nielsen an
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62 Lifetimes of molecular negative
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76 REFERENCES [19] V. V. Petrunin e
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78 REFERENCES [66] F. Robicheaux, P
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80 Chapter 5. Femtosecond VUV core-
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Page 106 and 107: 96 Chapter 5. Femtosecond VUV core-
Page 108 and 109: 98 Chapter 5. Femtosecond VUV core-
Page 110 and 111: 100 Chapter 5. Femtosecond VUV core
Page 130 and 131: 120 REFERENCES [17] A. Cavalleri et
Page 132 and 133: 122 REFERENCES [61] R. J. Finlay et
Page 134 and 135: 124 REFERENCES [104]R.W.Joyner,inTh
Page 136 and 137: 126 REFERENCES [152] T.-C. Chiang,
Page 138 and 139: 128 Chapter 6. Two-colour pump-prob
Page 154 and 155: 144 REFERENCES [16] Information ava
Page 158 and 159: 148 The following three chapters ar
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