OSU 06/18/08 Ultrabroadband Rotational Spectroscopy: Novel Applications of a Shape Sensitive Detector BRIAN C. DIAN Purdue University Department of Chemistry.

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Presentation transcript:

OSU 06/18/08 Ultrabroadband Rotational Spectroscopy: Novel Applications of a Shape Sensitive Detector BRIAN C. DIAN Purdue University Department of Chemistry 560 Oval Dr, West Lafayette, IN Chandana Karunatilaka Post-Doc Amanda Shirar Graduate Student Giana Storck Graduate Student Kelly Hotopp Graduate Student Erin Blaze Biddle Undergraduate Ricky Crawley Jr. Undergraduate

OSU 06/18/08 Development of Ultrabroadband Microwave Techniques -Multi-octave coverage ( GHz) -Fast acquisition times (Full bandwidth in seconds or less) -High Sensitivity -Ultrashort pulse times (100 psec) -Relatively easy to couple in laser

OSU 06/18/08 Ultrabroadband Microwave Techniques Ideally Suited for Dynamical Studies -Complimentary to fluorescence- and mass-based detection methods -Molecular shape gives rise to a unique spectral signature -Spectrum  1/  r 2 (  = reduced mass) -Rotational transition moment relies on permanent dipole moment -Ideally suited to ‘dark’ spectroscopy

OSU 06/18/08 Our Current Experimental Focus -Excited state dynamics -Probe structural dynamics AFTER excited state processes (ISC, IC) occur -Amanda Shirar (RA02) -Characterization of combustion dyanmics -Build a molecular library of spectral fingerprints produced in discharge spectra -Giana Storck (RA03) -Development of ultrabroadband 2D rotational spectroscopy -Rotational analogs of NMR 2D techniques (COSY etc.) -Kelly Hotopp (RA13)

OSU 06/18/08 W W 0 0 Coupling Scheme 2 W W 0 0 Coupling Scheme 1 2-D DRS: Selective Excitation (Model Calculations) 0 ns 10 ns 20 ns 30 ns 40 ns 0 ns 10 ns 20 ns 30 ns 40 ns

OSU 06/18/08 Ultrabroadband MW Input Experimental Set-Up XYZ Translation Stage Pulsed Valve Manual Mini Balle-Flygare FTMW Cavity UV Input Supersonic Expansion Cools Molecules ~ 2 K UV Laser ~ 0.4 cm -1 Bw mJ nm Ultrabroadband Chamber Packed With Microwave Absorber

OSU 06/18/08 Cavity Setup MW Synthesizer Arb 12GHz Scope 50/ MHz 30 MHz +  30 MHz +  Generate Microwave Frequency Cavity Mixing Signal Detection - Molecular Frequency  - Frequency Shift 2Gs/s 100MHz Output Complete Phase, Frequency, Amplitude Control

OSU 06/18/ GHz PDRO 12 GHz Oscilloscope (40 Gs/s) 200W Arbitrary Waveform Generator 10Gs/s 100 MHz Quartz Oscillator GHz Chirped Pulse GHz 8-18 GHz Pulsed Sample Nozzle GHz GHz 1) 2) Interaction 3) Free Induction Decay Setup #1: Mix at 13GHz (Pulse Shaping) 20 dB 13.0 GHz PDRO

OSU 06/18/ GHz PDRO 12 GHz Oscilloscope (40 Gs/s) 200W Arbitrary Waveform Generator 10Gs/s 100 MHz Quartz Oscillator GHz Chirped Pulse GHz 8-18 GHz Pulsed Sample Nozzle GHz GHz 1) 2) Interaction 3) Free Induction Decay Setup #1: Mix at 13GHz (Pulse Shaping) 20 dB 13.0 GHz PDRO

OSU 06/18/08 Full Sweep Time DomainFull Sweep Frequency Domain Time and Frequency Domain Pictures of Ultrabroadband MW Pulses: Mix Off 13 GHz

OSU 06/18/08 FROG: 1 ns Sinc Pulse Mixed with 4 GHz sine wave on 10 GHz Carrier

OSU 06/18/ GHz PDRO 12 GHz Oscilloscope (40 Gs/s) 200W Arbitrary Waveform Generator 10 Gs/s 100 MHz Quartz Oscillator GHz Chirped Pulse GHz GHz Pulsed Sample Nozzle GHz 1) Detection 2) 3) Free Induction Decay Set Up 2: x4 Frequency Stretcher x4 20 dB 40 dB LNA: NF ~1.2

OSU 06/18/08 Time and Frequency Domain Pictures of Ultrabroadband MW Pulses: x4 Frequency Stretch Full Sweep Frequency Domain Full Sweep Time Domain

OSU 06/18/08 Low Order Harmonic Distortion from Quadroupler Frequency Resolved Optical Gate (FROG) Chirped Pulse (Linear frequency sweep) Harmonic Distortion from Arb. High Order Harmonic Distortion (Aliased) Signal

OSU 06/18/08 Phase Control Phase of the excitation pulse is imprinted on the molecular emission

OSU 06/18/ GHz PDRO 12 GHz Oscilloscope (40 Gs/s) 200W Arbitrary Waveform Generator 100 MHz Quartz Oscillator Pulsed Sample Nozzle GHz GHz 1) 2) Interaction 3) Free Induction Decay x4 20 dB How Do we Do This? Condensed Circuit Diagram GHz Chirped Pulse GHz GHz

OSU 06/18/ GHz PDRO 12 GHz Oscilloscope (40 Gs/s) 200W Arbitrary Waveform Generator 100 MHz Quartz Oscillator Pulsed Sample Nozzle GHz GHz 1) 2) 3) Detection Free Induction Decay x4 20 dB How Do we Do This? Condensed Circuit Diagram GHz Chirped Pulse GHz

OSU 06/18/08 Ground State Spectrum of 1-chloro-1-flouroethylene 476 lines assigned to date ~ 18,000:1 S/N across entire bandwidth (rms) ~12,000:1 S/N (Pk to Pk) Lines split by nuclear hyperfine of Cl Background subtracted with valve off 13 C fit in natural abundance Details RH14 35 Cl 37 Cl Hotband *H.M. Pickett, J Mol Spec. 148 (1991) 371.

OSU 06/18/08 Summary -Dual Cavity/CP-FTMW Setup -Two CP-FTMW generation schemes -Mix off of 13 GHz (Pulse Shaping) -X4 Frequency Stretch (General Excitation) -Complete Amplitude, Frequency, and Phase control of excitation pulse -Ultrashort pulse times (1ns or less) -Well suited for dynamical measurements

OSU 06/18/08 Acknowledgements Funding: Purdue University Camille and Henry Dreyfus Young Faculty Award ACS Petroleum Research Foundation Chandana Karunatilaka: Post-Doc Amanda Shirar: Graduate Student Giana Storck: Graduate Student Kelly Hotopp: Graduate Student Erin Blaze Biddle : Undergraduate Ricky Crawley Jr.: Undergraduate Students:

OSU 06/18/08