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Discussion of measurement methods for femtosecond and attosecond pulses
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Duration & Phase Long pulse = one color Short pulse = many colors; perfectly synchronized. 0.7 1.3 This is mathematical. It cannot be avoided
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What is fast enough for measurement? Streak Camera (currently ~500 fs) ½ ns Produce photoelectron replica Rapidly changing field Space charge, operating over many nanoseconds is a problem photocathode
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Measuring femtosecond pulses Why not ask the pulse to measure itself! c c x or c t Transmission, Fluorescence, Ions, Electrons, Diffraction question: What can be used for mirrors and beam splitters? What can be the nonlinear medium for attosecond pulses?
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Attosecond pulses were generated using laser fields and electrons (Why not use the streak camera?) 1.Photoionization 2.Use the pre-existing re-collision electron replica
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Laser fields easily push electrons around Making single attosecond pulses --- controlling the laser field 1 fs
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Atomic ionization produces a replica photoelectron pulse V 1/2 mV 2 = x - IP Measurement of the photo-electron replica is a measurement of the pulse
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F=ma once again linear polarization initial velocity (V 0x, V 0y, V 0Z ) V drift, x = V 0x - {V d = qE 0 (t)/m Sin ( t I + )} V drift, y = V 0y V drift, z = V 0z Drift velocity distribution Polarization
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A single sub-cycle X-ray pulse VxVx VyVy --- photoelectron replica is streaked (attosecond streak camera)
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Streaked photoelectron of 100 eV pulse -- parallel observation 70 attosecond I = 6x10 14 W/cm 2
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30 Å gg c =a(k)e ikx-i t Attosecond pulses are generated by a pre-existing photoelectron replica
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We need to do a similar thing to the pre-existing replica A (weak) 2 2 field breaks symmetry, generating even harmonics Each moment of birth (re-collision) has an optimum phase difference ( ) between and 2
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60 BBO /2 Wave plate Supersonic gas jet Experimental Set-Up calcite glass Ti:sapphire amplifier 1mJ, 27 fs @ 50 Hz grating MCP
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16 18 20 22 24 26 Harmonic order Delay [fs] What Phase difference moves the interferometer arms optimally?
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Re-collision time [rad] (t) Harmonic number (N ) Attosecond Temporal Phase Gate d ,2 (t) ~ d (t) e i (t) SFA : two color delay which maximizes the even harmonic signal
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Electron Wave-Packet Reconstruction Re-collision time [rad] Short trajectories Long trajectories Harmonic order SFA Electron wave packet measurement is equivalent to a xuv pulse measurement up to the transition dipole.
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Discussion of Orbital Imaging What are the meausred quantities?
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High Harmonics/Attoseconds pulses d(t)={ ra(k)e ikx d 3 r} e i{(IP+KE)t + } d(t) is essentially the Fourier transform of the wave function
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Transient alignment of molecules time
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The Experiment “Pump” Alignment pulse “Probe” HHG pulse (60fs, 5 x 10 13 W/cm 2 ) (30fs, 1.5 x 10 14 W/cm 2 ) H15 23.3eV H21 32.6eV H27 41.9eV H33 51.2eV H39 60.5eV Space Ti:sapphire CPA 1 TW, 27 fs @ 50 Hz
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Angle Dependent High Harmonic Spectrum
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Harmonics from N 2 and Ar 2 d( )= 2 a(k) g re ikx dx Note the relation to Photoelectron spectroscopy
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Normalized Harmonic Intensities Harmonic intensities from N2 at different molecular angles ELEL
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Reconstructed N 2 g Orbital Reconstructed from 19 angular projections wave function, not its square We see electrons! Amplitude and Phase!
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Final comment: Another perspective on the re-collision electron The probability of the electron being driven back is 50% The area of the electron wave packet when it returns is ~(10 Angstroms) 2 The time window is about 1 femtosecond Charge per unit area per unit time is current density. J~10 11 Wcm 2. This is a truly phenomenal number--- the electron can hardly miss. Why not allow it to diffraction from the molecule?
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