Coherent Phase Control of Electronic Transitions in Gallium - - PowerPoint PPT Presentation

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Coherent Phase Control of Electronic Transitions in Gallium - - PowerPoint PPT Presentation

Coherent Phase Control of Electronic Transitions in Gallium Arsenide Robert J. Gordon, Sima Singha, and Zhan Hu Department of Chemistry University of Illinois at Chicago FRISNO 11 Aussois, France March 31, 2011 Passive Control F. Crim


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Coherent Phase Control of Electronic Transitions in Gallium Arsenide

Robert J. Gordon, Sima Singha, and Zhan Hu Department of Chemistry University of Illinois at Chicago

FRISNO 11 Aussois, France March 31, 2011

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SLIDE 2
  • F. Crim

Passive Control

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SLIDE 3

Active Control

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SLIDE 4
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SLIDE 5

Outline

  • Motivation and methods
  • Results from open loop experiments
  • Results from closed loop experiments
  • Proposed mechanism
  • Conclusions
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SLIDE 6

Cut in Decemet’s Membrane

6 ns, 1064 nm

30 ps, 1064 nm

Vogel, et al., Invest. Ophthalmol. Vis. Sci. 35, 3033 (1997)

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SLIDE 7

Surface Modification with Ultrafast Pulses

Stoian, et al., Appl.Phys.

  • Lett. 80, 353 (2002)
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SLIDE 8

SEM images of the ablation craters on GaAs

1, 5 and 5+1 pulse trains

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SLIDE 9
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SLIDE 10
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SLIDE 11

Outline

  • Motivation and methods
  • Results from open loop experiments
  • Results from closed loop experiments
  • Proposed mechanism
  • Conclusions
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SLIDE 12
  • Phys. Rev. B 82, 115205 (2010)

LIBS/Photoluminescence Spectrum

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Effect of Laser Polarization

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SLIDE 14

PL Signal at 450.8 nm

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SLIDE 15

Control Landscape

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Effects of Polarization and Incidence Angle

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SLIDE 17

Effect of Laser Fluence

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SLIDE 18

Effect of Laser Phase

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SLIDE 19

Outline

  • Motivation and methods
  • Results from open loop experiments
  • Results from closed loop experiments
  • Proposed mechanism
  • Conclusions
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Closed Loop Control

Sine phase optimized for 390-450 nm sine phase optimized for 420-440 nm random phase optimized for 390-450 nm

  • J. Phy. Chem. A (in press)
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SLIDE 21

20100528-115537 PRB paper graph

Optimum Pulse Shapes for Open and Closed Loops

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Effect of Laser Fluence

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Effect of Laser Polarization on Optimized PL Spectrum

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Effect of Laser Phase on Open-Loop Spectrum

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Effect of Laser Phase on Closed-Loop Spectrum

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Outline

  • Motivation and methods
  • Results from open loop experiments
  • Results from closed loop experiments
  • Proposed mechanism
  • Conclusions
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Mechanistic Questions

  • Where does the new band come from?
  • How is it possible to excite optical

phonons at fluences above the threshold for melting?

  • How does light couple to the plasma?
  • How does energy couple to the phonons?
  • Where does the coherence come from?
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SLIDE 28
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Ratio of double pulse to single pulse fluorescence as a function of delay time and total energy

Si<111>

  • App. Phys. Lett. 90, 131910 (2007), J. Appl. Phys. 104, 113520 (2008)
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SLIDE 30
  • Dispersion relation for

a light wave in a plasma:

  • Critical density:
  • Index of refraction:
  • Total reflection:

pe L L pe L

c k ω ω ω ω ≥ ⇒ + =

2 2 2 2

2 2

4 e m n

L e cr

π ω =

2 2 2

1 1

L pe cr e

n n n ω ω ε − = − = =

θ θ ε

2 2

cos ; sin ) (

cr e

n n z = =

Light Propagation in a Plasma

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SLIDE 31

Brunel or vacuum heating

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Comparison of Closed and Open-Loop Pulses

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Conclusions

  • Coherent control of carrier recombination was achieved

at fluences well above the damage threshold.

  • The primary mechanism for open loop control appears to

be phonon-hole scattering, with trapping of carriers in the L-valley.

  • Brunel (ponderomotive) heating launches ballistic

electrons that excite the phonons.

  • Effect of laser phase suggests a competition between

photoemission and phonon excitation.

  • Random phase optimization appears to converge to a

different control pathway.

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SLIDE 34

YaomingLu, Youbo Zhao, Slobodan Milasinovic John Penczak, SimaSingha, Zhan Hu

Supported by NSF, USAF Surgeon General, UIC

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( ) ( )

[ ]

ϕ π ω ψ + − = T m m A / 2 sin

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Time Delay Scans

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Properties of the Optimum Pulse vs. Fluence