vishnu vardhan krishnamacharipotma/vishnu060206.pdf · 2006. 6. 23. · vishnu krishnamachari group...

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BERKELEYDAVISIRVINELOS ANGELESMERCEDRIVERSIDESAN DIEGOSAN FRANCISCOSANTA BARBARASANTA CRUZ Department of Chemistry UNIVERSITY OF CALIFORNIA, IRVINE Vishnu Vardhan Krishnamachari Heterodyne CARS imaging: First results Group Seminar June 2, 2006

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  • BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    Vishnu Vardhan Krishnamachari

    Heterodyne CARS imaging:First results

    Group SeminarJune 2, 2006

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    Contents

    CARS is not Raman!

    Heterodyne CARS

    Experimental setup

    DMSO-Glass Experiment

    Contents

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    CARS is not Raman!

    Frequency dependence of third-order non-linearsusceptibility around a Raman transitionRaman

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    CARS is not Raman!

    Spontaneous Raman emission intensityRaman

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    CARS is not Raman!

    CARS intensity : Single peak

    CARS

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    CARS is not Raman!

    CARS intensity : Double peak

    CARS

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    CARS is not Raman!

    CARS intensity

    Non-resonant and resonant signals interfere

    Difficult to analyze the spectrum

    Huge background => Poor SNR & sensitivity

    CARS intensity is not proportional to the concentration

    CARS

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    Heterodyne CARS

    Heterodyne detection:Detection of the desired signal by mixing it with a“known” or “well-characterized” signal.

    HeterodyneCARS

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    Heterodyne CARS

    ωCARSωlo

    Detector

    • Δφ = π/2 ⇒ Ιout∝ Im{χ(3)}

    ∝ Conc • Δφ = 0 ⇒ Ιout∝ Re{χ(3)}

    HeterodyneCARS

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    Experimental Setup

    Setup

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    Experimental Setup

    Setup

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    DMSO Interference

    X

    Y

    X0

    Interference between local oscillator and CARS signal

    Results

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    DMSO Interference

    Time

    X0

    Interference between local oscillator and CARS signal

    Results

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    DMSO-Glass Experiment

    Glass DMSO

    + local oscillator

    t

    X0

    Simultaneous observation of two heterodyne signals

    Results

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    DMSO-Glass Experiment

    Amplitude of oscillation

    Phase difference

    Results

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    DMSO-Glass Experiment

    Results

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    DMSO-Glass Experiment

    Results

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    DMSO-Glass Experiment

    Discrepancies

    Results

  • Vishnu Krishnamachari Group Seminar: June 2, 2006

    Contents

    Raman

    CARS

    HeterodyneCARS

    Setup

    Results

    BERKELEY•DAVIS•IRVINE•LOS ANGELES•MERCED•RIVERSIDE•SAN DIEGO•SAN FRANCISCO•SANTA BARBARA•SANTA CRUZ

    Department of ChemistryUNIVERSITY OF CALIFORNIA, IRVINE

    Conclusion

    Raman versus CARS

    Non-resonant background and its role

    CARS intensity is not proportional to conc.

    CARS Heterodyne setup

    Experiments with DMSO + Glass