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Ultrafast Laser Ablation and Plasma Diagnostics. Zhiyu Zhang Center for Ultrafast Optical Science Department of Electrical Engineering and Computer Science University of Michigan, Ann Arbor, MI. Outline. Introduction and Motivation
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Ultrafast Laser Ablation and Plasma Diagnostics Zhiyu Zhang Center for Ultrafast Optical Science Department of Electrical Engineering and Computer Science University of Michigan, Ann Arbor, MI
Outline • Introduction and Motivation • Multi-diagnostic comparison of plasmas by ultrafast laser and nanosecond laser ablation • Multi-pulse ablation • Application of double and multi-pulse ablation: isotope enrichment and clusters formation • Summary
Ultrafast Laser Applications: Materials Processing (I) Above Ablation Threshold • Micromachining: metal, semiconductor, dielectric, dental tissue, 100nm lateral, 10nm vertical; Appl. Phys. A 68 369, Appl. Phys. A 68 403 • DNA transfection; Nature 418 290 • Patterning biomaterials; Appl. Surf. Sci. 208-209 245 • Fresnel zone plate fabrication; Opt. Exp. 10 978 • Surface microstructureing; APL 81 1999 • Photomask repair; J. Vac. Sci. Technol. B 21 204
Ultrafast Laser Applications: Materials Processing (II) Below Ablation Threshold • Waveguide direct writing; Opt. Lett. 21 1729 • Phase transition; JETP Lett. 76 461 • 3D micro-photopolymerization; Nature 412 697 • Nonlinear optical coefficient enhancement; APL 81 1585 • Precipitating nanoparticles inside glasses; APL 81 3040
SnO2 R-cut Al2O3 Ultrafast Laser in Materials Processing
100 fs 100 MHz 2 nJ X 106 0.5 mJ Oscillator Regen Amplifier Nd:YAG 200 mJ Argon 4-pass Amplifier 2-pass Amplifier Compressor 20 mJ 100 fs 10 Hz 100 mJ Nd:YAG Ultrafast Laser System 10 Hz X 10,000 200 ps Beam Splitter Stretcher
Ultrafast Laser System 100 fs 10 Hz 100 mJ
High-Repetition Rate Commercial Ultrafast Laser Laser: 1 kHz, 1 mJ/pulse, 150 fs
Plasma Plume Imaging & Spectroscopy Langmuir Probe • 2” Substrate Holder: • temperature: 77 K to 1000°C • rotation & translation • bias: 0 to -500 V HeNe Electrostatic Analyzer (charge state & energy) Lasers: 10 Hz 780nm 110fs Multi-Target Selector(4 targets with rotation) or Dt Position Detector Vacuum: 10-9 Torr Experimental Setup
MCPs – straight • i/o • Vb • +Vs • Va • - Vs MCPs curved sector • Einzel • lens Electrostatic Energy Analyzer Select ions with E/q=2.254 Vs
Time-of-Flight Spectrum: BN Laser: 100 fs, 780 nm, 50 J/cm2
Time-Resolved OESAl Ablated with 100-fs Pulses • 100 ns Delay Increment • 50 ns Acquisition Window • 100, 780nm, 1J/cm2 Laser Pulses • Continuum Emission at Early Time
Langmuir Probe I-V Curve • Plasma parameters related to the different regions of the I-V curve • Probe theory developed to extract the parameters from the I-V curve • Time-resolved analysis (1ms resolution)
HeNe Probe Laser Deflection Plume Quad Detector Vout HeNe j: Ion or Neutral component Self-similar expansion model for both ion and neutral species C.L. Enloe et al,Rev. Sci. Instrum. 58, 1597 (1987)
Plasma 0 Neutrals HeNe Deflection Signal BN Ablation: 6ns, 18 J/cm2 Parameters: Vion 4.76x106cm/s Vneutral 1.04x106cm/s Nion 5x1014 Nneutral 1x1017
In-situ Analysis Plasma Diagnostic Technique • Electrostatic Energy Analyzer • Charge state, Ion energy distribution • Langmuir Probe • Electron temperature, Plasma and floating potential, Density of electrons and ions • Spatial and temporal resolution (1ms) • Optical Emission Spectroscopy • Plasma temperature, Excited states • ns time resolution • Laser Deflection Probe • Ion to neutral ratio • Hydrodynamic component Target: Metal (Al), Nitrides (BN), Oxide (SnO2)
Energy Spectrum of AlEffect of Laser Pulse Width 6 ns,1.06 mm 1.3J/cm2 80 fs, 780 nm 0.4J/cm2 Al Target Ablated in Vacuum
Time-Resolved Electron Temperature: Optical Emission Spectroscopy • Laser Pulses: • 6ns • 1.06mm • 1.4J/cm2 • 100fs • 780nm • 0.4J/cm2
Time-Resolved Electron Temperature: Langmuir Probe 6 ns 80 fs Laser pulses: 80fs 780nm 0.4J/cm2 6ns 1.06mm 1.3J/cm2 Langmuir Probe: 10cm away from Al target
HeNe Deflection: Ion to Neutral Ratio 100 fs Laser Neutral Energy:4 eV Ion Energy: 85eV 6 ns Laser Neutral Energy:4 eV Ion Energy: 100eV
Plume Properties Modified by Laser Pulse • Pulse width: plasma shielding and heating effects • Pulse contrast: enhance the high energy component in the plume (Appl. Surf. Sci 2000) • Pulse intensity: optimum ablation efficiency (MRS 2002) • Multi-Pulse: enhanced ion properties (APL 2003)
Ion Yield and Energy in Ablation Plumes 3.3kJ/cm2 • 10Hz • Ti:Sapphire • Same focus spot • Varying pulse • energy • Ion Energy is converted from TOF signal 0.8kJ/cm2
Laser Wave in Plasma ncr Light Wave in Inhomogeneous Plasma s-pol: Collisional absorption p-pol: Collisional + Resonance absorption Collisional absorption Resonance absorption w ~ laser frequency L ~ plasma scale length v*ie ~ electron-ion collision frequency c ~ speed of light
Modify the Ablation Dynamics by Double Pulse Ablation • Saturation of absorption occurs as single- pulse energy increases due to plasma reflection • Use an appropriately time-delayed secondary laser pulse to add energy into the plasma during the early stages of its expansion. • Examine the effect on the plasma and the clusters
Double pulse experiment • Initial gradient scale length of a plasma Two identical 300fs pulses: tens of ps delay Ref: C. Y. Cote et. al Phy. Rev. E 56, 992 (1997 ) • Thin Film Deposition: reducing particulate CO2 and YAG lasers: 4ns delay Ref: S. Witanachchi, et. al Appl. Phys. Lett. 66 1469 (1995) • X-ray emission Weak pre-pulse, 2ns delay Ref: H. Nakano et. al Appl. Phys. Lett. 79 24 (2001)
Time-of-Flight: Single vs. Double-Pulse Laser: 110fs, 780nm, p-polarized 1x1016 W/cm2 0~50ps 2x1016 W/cm2
Double-Pulse Enhanced Optical Emission Laser: 130fs, 780nm, p-pol 1x1016 W/cm2 0~50ps
Langmuir Probe: Double-Pulse Enhanced Ion Density Laser: 130fs, 780nm, p-pol 1x1016 W/cm2 0~50ps
Charge State Distribution: Single vs. Double-Pulse Average Charge: Single: 2.5 Double 5-ps: 3.1 Double 10-ps: 3
Ion Yield vs. Laser Intensity (Double-Pulse) Maximum Intensity: 1x1016 W/cm2
RC M3 M4 BS BS RC RC BS RC 2 M1 M2 4 1 3 Original Beam Path Setup for Generation of 4-pulse Sequence
t1 t1 t3=t2 - t1 t2 Silicon Ablation by Multi-pulse Laser Intensity: 5x1015 W/cm2 Four-Pulse: t1=5ps, t3 is a variable
Isotopic Enrichment: Double-Pulse Enhancement BN Ablation – 120 fs, 2 x 1016 W/cm2, Dt = 10 ps Isotope Ratio Ion Yield
Time-resolved Magnetic Field Magnetic field by RA Laser Intensity: 1x1016 W/cm2 Toroidal magnetic field Laser Intensity: 5x1018 W/cm2 Borghesi et.al. PRL v81,p112 Sandhu et.al. PRL v89,p225002
Questions • Cluster component in the plume? • Surface roughness is caused by growth effect or clusters formed in plume? • High intensity femtosecond plasma bursts result in dense cluster formation?
Cluster Formation for Cu/NiLaser intensity = 2 x 1016 W/cm2 ; Tm ~ 1300 C
Cluster Size Distribution: Ni Ni: RT, 10Hz Laser, Single Pulse, 2x1016W/cm2 Average Size: 242 nm +155nm
Cluster Size Distribution: Ni Ni: RT, 10Hz Laser, Double Pulse, 1x1016W/cm2, 5ps Delay Average Size: 99nm+41nm
Cluster Size Distribution: Ge Single full-energy pulse
Cluster Size Distribution: Ge Double pulse
Clusters Formation Mechanism (I) • Condensation of ns laser ablation plume • High background pressure, 1 ~ 10 Torr • Hydrodynamic expansion and thermodynamic condensation • Plume nonuniformity gives cluster size distribution • Average size: less than 10 nm
Clusters Formation Mechanism (II) • Photomechenical Effects - fragmentation • Clusters are formed by fragmentation due to the strain associated with gradient of expansion velocity • Cluster size determined by fragmentation time • Average size: less than 10 nm for 1ps fragmentation time
Clusters Formation Mechanism (III) • Photothermal Effects – phase explosion • Superheating leads to homogeneous nucleation • Mixture of vapor and liquid forms clusters • Average size: possible ~100 nm
“Femto-Jet” nozzle Hagena Equation Femtosecond laser ablation: P0: 103 ~104 atm a: small, supersonic expansion Density: very large; k: large for heavy atoms d: jet throat diameter a: jet expansion half angle p0: backing pressure T0: initial gas temperature k: material dependent constant number of atoms per clusters: Nc (G*)2.0~2.5