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Molecular excitation by chirped laser radiation in ladder climbing and autoresonance regimes
Gilad Marcus, Arie Zigler and Lazar Friedland Racah Institute of Physics, Hebrew University, Jerusalem, Israel
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Outlines for the Lecture
Definition of the problem Ladder climbing and the Auto-Resonance concepts Ladder-climbing experiment on HF molecule Radiation source for Excitation of the molecule
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Basics of Auto-Resonance
Harmonic Oscillator Anharmonic Oscillator
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Pendulum frequency Vs. amplitude
w/w0 [q/p]
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How to excite nonlinear systems into high energy ?
Changing the drive frequency will keep it in resonance. Pendulum frequency Vs. amplitude [q/p]
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How to excite nonlinear systems into high energy ?
Changing the drive frequency will keep it in resonance. but we also have to continually adjust the phase
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Few method to excite nonlinear oscillator
Feedback control. (requires a real time feedback) Exact tailoring of the force. (requires pre-knowledge of the system) Ladder-climbing & autoresonance
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Auto-Resonance The drive frequency is slowly changed
(slow chirp) The oscillator is automatically phase locked (provided that the force exceed a certain threshold) The energy of the oscillator is a function of the drive frequency
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Threshold-chirp relation
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Auto-Resonance simulation
wdrive=w0-at Amplitude, a Phase Mismatch F { L. Friedland et al. Phys. Plasmas. 5 (645) }
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Ladder climbing in a quantum systems
Morse Potential D Energy levels in Morse potential. Ladder of energy levels with decreasing gaps.
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Two levels with constant frequency drive
constant frequency drive force
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Two level with chirped drive
Efficient conversion when Ts / TR=2.8 Ts / TR=1 chirped drive force time
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The validity of the two level approximation
Which means – the width of resonance is small enough to include only two levels
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Characteristic times
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The limit between quantum mechanics and classicality
In terms of the three characteristic times:
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The condition for efficient ladder-climbing
In terms of the three characteristic times:
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Efficient classical autoresonance
. In term of the characteristic times:
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P1-P2 parameters Quantum limit: Efficient transfer between 2 levels:
Efficient Autoresonance:
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P1-P2 parameters .
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Ladder climbing-below threshold
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Ladder climbing-above threshold
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Autoresonance-below threshold
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Autoresonance-above threshold
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Design consideration for experiment
.
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Experiment with HF molecule: requirements from the radiation source
In the IR regime To bring the population to the 4th level Ladder climbing threshold
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Theoretical curve of phase matching for PPKTP with period of 27
Theoretical curve of phase matching for PPKTP with period of 27.1m pumped by wide-band Ti:Sapphire Laser Idler spectrum 2-3m Signal spectrum 1-1.5m
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The Experiment Collimated Ti:Sapphire
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The Signal & Laser spectrum
Signal spectrum O Non collinear --- Collinear
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Delay as a function of wave-length
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Chirp measurement
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IR specifications Bandwidth – 25% Pulse length – 185 psec
Spot size 60m x 700m Energy – up to 200mJ
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P1-P2 parameters - Witte et al. – Cr(CO) 6 - Maas et al. - NO
- Our experiment - HF .
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Demonstration of ladder climbing on HF molecule.
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IR spectrum
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HF experiment results Standard deviation Avg. Number of photons
Conditions: 4.6 11.16 10 torr HF 0.7 0.5 10 torr Air 0.57 0.33 Continually evacuated 1.1 1.5 10 torr HF & filtered spectra
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Summary We have shown theoretically a smooth transition from ladder-climbing to autoresonance We have generated a chirped, ultra wideband radiation source in the IR We have demonstrated ladder-climbing on HF molecule
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Plans for the future Improving the optics to allow us to be above the threshold Check the transition from quantum-mechanics to classicality. Other molecules
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The end
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