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HIGH-RESOLUTION COHERENT THREE-DIMENSIONAL SPECTROSCOPY OF IODINE
ZURI HOUSE, PETER C. CHEN, THRESA A. WELLS
SPELMAN COLLEGE, ATLANTA GA
BENJAMIN R. STRANGFELD
GEORGIA INSTITUTE OF TECHNOLOGY, ATLANTA GA
OUTLINE/PURPOSE
• Background
• Experimental Set-up
• Four Wave Mixing Processes
• Data Analysis
• Next Step
• Conclusion
• Acknowledgements
• Purpose of Experiment: To explore and test a new 3 dimensional technique on Iodine
BACKGROUND- IODINE• Purpose of the study
• Understand how 3D spectroscopy can be used for molecules without known spectroscopic constants
• Establish a standard procedure for analyzing unknown molecules
• Reasons for choosing iodine
• Energy levels for two states involved are known and thoroughly studied (X to B transition)
• Simple diatomic molecule with no isotopomers• Used low resolution absorption spectrum to determine
roughly where to set laser
BACKGROUNDTypes of Spectroscopic Methods
• Raman, IR, UV-Vis, NMR (a few examples)
Characteristics of Techniques (in heavily congested systems)
• 1D- highly congested 2D- less congested
• 3D- even less congested, and selective (see next slide)*2D and especially 3D techniques are new and innovative
. .
λaλa
λbI
RESONANCE• 3D spectroscopy is a fully resonant process
• When 3 beams are resonant with the levels in the molecule, a lot of light is generated and the peaks are more intense
• triply resonant features are more intense than > doubly > Singly
i ii iii iv
532 M S ω4 M 532 S ω4 M S 532 ω4 532 S M ω4
ω4= ω532- ωS + ωM
• Non-linear optical process• Can only be done with very intense (pulsed) lasers• Taking 3 beams and overlapping them to create a new 4th
beam that has its own wavelength (determined by molecule present)
• Detected by monochromator• Which process is responsible for my results?
FOUR WAVE MIXING PROCESS
EXPERIMENTAL SET-UP
3 lasers used for the Four Wave Mixing Process• Mopo (tunable)• Sopo (broadband OPO)
• Can adjust to find fully resonant peaks• 532nm ND: YAG laser
• Wavelength cannot be changed• Selects J value, primarily vibrational changes
532nm Nd: YAG Laser (GCR)
532nm Nd: YAG Laser (GCR)
532nm Nd: YAG Laser
SampleRaman Shifters
SOPO
Monochromator with CCD
MOPO
532 S M ω4
SLOPE OF THE LINE
Slope of lines
• The slope of the line which passes through all of the clusters in that particular area in the pattern was derived
• Slope should be 1 because the axes are ω4 vs. ωM
• Derivation from equation ω4 = ω532- ωS + ωM to y=mx+b
1.ω4 – (ω532 – ωS) = ωM
2.ωM = ω4 + (ωS – ω532)
y = mx + b• Used to help determine spectroscopic constants
VERTICAL SPACING
Intercluster Relationship
• Indicates spacing between the excited levels within the B-state
• Since levels are relatively evenly spaced, levels are not approaching the dissociation limit for the B-state
DIAGONAL SPACING
Intercluster Relationship
• Tells us about the spacing between the excited levels within the higher X-state
• Aren’t converging, so dissociation level hasn’t been reached• All of this information determined is electronic and vibrational
• Next: find rotational information (intracluster relationship)
FURTHER STUDY• Use simulation (via Excel spreadsheet) to:
• Tune the laser to a specific resonance and decrease the bandwidth to control the number of peaks within a cluster
• Employ same techniques Benjamin Strangfeld described and calculate B’s for designated triangles within a cluster
• Compare coherent 3D spectroscopic constant to literature values
ACKNOWLEDGEMENTS
Peter Chen
Thresa Wells
Benjamin Strangfeld
Aspiring Researchers Program
NSF Grant: NSF CHE-0910232