The measured electronic transitions on the OH proved the functionality of our precision spectroscopy laser system and demonstrated the successful detection of the molecules in the vibrational ground state v00 = 0. This thesis contains the groundwork for future measurements of vibrational transitions of the OH molecule. The required mid IR optical parametric oscillator (OPO) has been built in this thesis. Improving its tunability and implementing a phase-locked loop (PLL) to stabilize it to the optical frequency comb (OFC) is the next step. Once this is accomplished, we plan to observe vibrational
one-photon or two-one-photon transition in OH at 2.7µm or 2.9µm, respectively.
Other molecular systems might also be worth considering. Both the OPO and the dye laser have a wide tuning range, which makes them applicable for a variety of different molecules. In general, the simplest molecules are of greatest interest for testing the standard model of physics. Ab initio calculations are more likely to match experimental precision if the system contains as few electrons as possible. Thus, the H2 molecule is the perfect candidate for high-resolution spectroscopy of vibrational transitions.
The challenge of measuring vibrational transitions of the symmetric H2 molecules is the zero dipole moment, since we require a non-zero dipole moment for a one-photon electric dipole transition. One solution might be Raman spectroscopy, which is based on the
11.2. Beyond the Electronic Excitation of OH difference frequency of two electric fields. This principle also applies for one static field with zero frequency and a second field supplied by the IR OPO. In this case, the constant field induces a dipole moment and allows excitation in the IR. An even more straightforward approach might be a measurement of the HD molecule, which is asymmetric and has a small but non-zero dipole moment without further manipulations. The main change that would need to be made spectroscopy on H2 or HD is the implementation of a resonance-enhanced multiphoton ionization (REMPI) setup including a mass spectrometer for detection.
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Abbreviations
AC alternating current
AlGaInP aluminium gallium indium phosphide AOM acoustic-optical modulator
AR anti-reflective AVAR Allan variance BBO beta barium borate
BIPM bureau of weights and measures
CIPM international committee for weights and measures CORDIC coordinate rotation digital computer
CW continuous wave
DC direct current
DFB distributed feedback
DFG difference frequency generation ECDL external cavity diode laser EDM electric dipole moment EMF electromotive force EOM electro-optic modulator ERF error function
FEM finite element method FFT fast Fourier transform FM frequency modulation
FPGA field-programmable gate array FPI Fabry-Perot interferometer FSR free spectral range
FT Fourier transform
FWHM full width at half maximum GMT greenwich mean time
GNSS global navigation satellite system GPS global positioning system
HR high-reflective
HV high voltage
IR infrared
IUPAC international union of pure and applied chemistry LHC large hadron collider
LIF laser induced fluorescence
LISA laser interferometer space antenna MBD maxwell-boltzmann distribution MDEV modified Allan deviation
MPI multiphoton ionization
MTS modulation transfer spectroscopy MVAR modified Allan variance
Nd:YAG neodymium-doped yttrium aluminum garnet NIST national institute of standards and technology NPRO non-planar ring oscillator
NTC negative temperature coefficient OD deuterated hydroxyl radical OFC optical frequency comb OH hydroxyl radical
OPA optical parametric amplification OPO optical parametric oscillator PBS polarizing beam splitter PCF photonic crystal fiber
PD photodiode
PDH Pound-Drever-Hall PEEK polyether ether ketone PI proportional-integral
PID proportional-integral-derivative PLL phase-locked loop
PMM phase mismatching PMT photomultiplier tube
PPLN periodically-poled lithium niobate PPM perfectly phase matched
PPS pulse per second
PTFE polytetrafluoroethylene PVAR parabolic variance PVC polyvinyl chloride PWM pulse-width modulation PZT piezoelectric transducer
QM quantum mechanical
QPM quais phase matching
Chapter 11. Abbrevations
RAM residual amplitude modulation
REMPI resonance-enhanced multiphoton ionization RFT rotating-frame transformation
RMS root-mean-square
RTD resistance temperature detector RWA rotating-wave approximation SAW surface acoustic wave
SFG sum frequency generation SHG second-harmonic generation
SM standard model
SNR signal to noise ratio SSE sum of square errors TAI international atomic time TB thermal background
TDLAS tunable diode laser absorption spectroscopy TEC temperature controller
TEM transverse electromagnetic mode TOF time-of-flight
TTL transistor-transistor logic UHV ultra-high vacuum
ULE ultra-low expansion
USNO united states naval observatory UTC coordinated universal time
UV ultraviolet
VCXO voltage-controlled crystal oscillator WM wavelength modulation
YAG yttrium aluminum garnet
Acknowledgments
During the last couple of years, I worked side by side with great people. Foremost, I would like to especially thank Dr. Samuel Meek for inviting me into his group and providing excellent conditions for our work. I am grateful for his continuous support, mentoring, brilliant ideas in advancing the project and great motivational speeches.
Furthermore, I would also like to thank Prof. Dr. John Furneaux as a constant source of knowledge during my first year. Without his contributions, I probably would not have come this far.
A big thank-you goes out to Prof. Dr. Alec Wodtke for hosting our group and providing the best working environment possible. The laboratory I was allowed to work in was great, but the real treasures are the people, the group members at the university, as well the ones sitting at the MPI who I could ask anytime for advice, and it was provided.
I am also thankful to Tim Diedrich and Reinhard B¨ursing for technical suggestions to my drawings, moving them from good to excellent. As well I am thanking the mechanical workshop for transferring my drawings into precise physical objects.
I am especially thankful to Prof. Dr. Ansgar Reiners, who joined my thesis advisory committee and allowed me to enroll in the GAUSS program. Furthermore, I would like to thank Prof. Dr. Claus Ropers, Prof. Dr. Stefan Mathias, Prof. Dr. Dirk Schwarzer and Dr. Holger Nobach for being members of my examination board.
Sincere thanks are also given to all my colleagues, who helped me to clear my mind during a good game of table soccer, namely Marvin Kammler, Sven Kaufmann, Nils Hertl, Jascha Lau and Tim Diedrich. The order in this list does not reflect the skill level. You are all awesome!
Special gratitude goes to my parents, for their faith in me and providing the old sunflower Toyota, so I could swiftly move up the Fassberg. And last but not least Nora, you have my gratitude for your love, encouragement, and support. I’m grateful for the quality time together, and even more for your patience when I spent to little time with you.
Thank you all so very much.