High-Harmonic Generation II

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Soft X-Rays and Extreme Ultraviolet Radiation High-Harmonic Generation II Phasematching techniques Attosecond pulse generation Applications Specialized optics for HHG sources Dr. Yanwei Liu, University of California, Berkeley and Lawrence Berkeley National Laboratory

Phase-matching of nonlinear process Growth of second-harmonic power in a crystal along the propagation direction, assuming a constant pump intensity. Solid curve: phase-matched case, with the power growing in proportion to the square of the propagation distance. Dashed curve: non phase-matched case, with the second-harmonic power oscillating between zero and a small value. Adopted from Encyclopedia of Laser Physics and Technology

HHG in Hollow Fibers

HHG in Hollow Fibers Phase-Matched Generation of Coherent EUV Radiation Andy Rundquist, et al. Science 280, 1412 (1998) No phase-matching, n = 23-31, EUV output beam Pressure phase matching With phase-matching, n = 23-31, EUV output beam

Fully coherent EUV from HHG in hollow fiber

Short Modulation Period Capillaries Extend Phase Matching from 85 ev (Unmodulated Fibers) to 160 ev A. Paul et al., Nature (2 Jan 2003) E. Gibson et al., Science (3 Oct 2003)

Coherent Soft X-Ray HHG with Quasi-Phase Matching C k filter Courtesy of E. Gibson, A. Paul, H Kapteyn, M. Murnane, and colleagues Science 302, 96 (3 Oct 2003)

Quasi phase matching using counter-propagating pulses Intensity Picosecond pulses, HHG coherence length ~ 1mm. X. Zhang, A. L. Lytle, H. C. Kapteyn, M. M. Murnane, O. Cohen, Nat. Phys. 3, 270 (2007).

Quasi phasematching using CW counter-propagating laser O. Cohen et al., Phys. Rev. Lett. 99, 53902 (2007).

The case for short pulses Attosecond physics F. Krausz, M. Ivanov Review of Modern Physics 81, 163 (2009) By Harold Doc Edgerton, MIT

Long (many cycles) pump laser generates attosecond pulse train 1.3 fs 2.7 fs

Isolated attosecond pulse generation using few-cycle pump Usually a multilayer to select high energies Intense peak generates highest photon energy Bandpass filter selects highest photon energy in a single attosecond pulse M. Hentschel et al., Nature 414, 509 (2001).

Carrier-Envelope Phase (CEP) of ultrafast pulse Cosine wave Sine wave

Cosine waveform generates single attosecond pulse A. Baltuska et al., Nature 421, 611 (2003); F. Krausz, M. Ivanov, Rev Modern Phy 81, 163 (2009)

While sine waveform generates two attosecond pulses A. Baltuska et al., Nature 421, 611 (2003); F. Krausz, M. Ivanov, Rev Modern Phy 81, 163 (2009)

Applications of HHG sources Merits of HHG source: Ultrafast EUV/SXR pulses Temporal resolution in fs/as scale, never reached before Molecular dynamics excited by EUV photons Inner-shell probe (high photon energy) Well-controlled pump-probe experiments (automatically synchronized with IR pump) Coherent radiation at short wavelengths (nm and fsec) Coherent Diffractive Imaging (CDI, or lenseless imaging) Holographic Imaging Zoneplate Imaging

Direct measurement of 750 nm light wave pulse duration A 250-as EUV pulse is used to map the electric field of 750-nm laser light wave 2.7 fsec/cycle 800 nm, 3 cycle, ~7 fsec Laser light Field, E L (f) EUV pulse Electron detector Electrons Atoms Field-induced charge of electron momentum, p(t) Overlap of 7 fsec IR pulse and 250 asec EUV pulse. EUV frees electrons, IR electric field accelerates these electrons. These electrons arrive in waves via time-of-flight tube to detector. E. Goulielmakis, et al. Science 305, 1267 (2004)

Unprecedented time resolution Photo electron yield Tungsten (W) Conduction Band electrons Shifted birth times Attosecond spectroscopy in condensed matter A. L. Cavalieri, et al., Nature 449, 1029 (2007)

Fs XUV transient absorption spectroscopy Orbital alignment and nonadiabatic behavior in the strong-field ionization of Xe Electromagnetically Induced Transparency (EIT) in the XUV via coherent coupling of He double excitation states EUV absorption EUV absorption EUV absorption EUV absorption EUV // IR EUV! IR Courtesy of Zhi-Heng Loh and Stephen Leone, Univ. Calif., Berkeley

EUV pump, EUV probe Electronic motion inside an atom (computational) Attosecond Pump Probe: Exploring Ultrafast Electron Motion inside an Atom S. X. Hu and L. A. Collins, PRL 96, 073004 (2006)

Zone plate imaging with femtosecond EUV pulses Jong Ju Park et al., "Soft x-ray microscope constructed with a PMMA phase-reversal zone plate," Opt. Lett. 34, 235-237 (2009) 30 fs, 0.6 mj n = 59 n = 61 Mo/Si multilayer n = 63 n = 65

Co-axial multilayer optics used in HHG pump-probe experiments from Dr. R. Kienberger M. Drescher et al., Science 291, 1923 (2001)

Reflectivity! " Bandwidth Multilayer mirrors depend on constructive interference from individual interfaces Higher reflectivity needs more layers Bandwidth gets narrower with more layers Attosecond pulse " Broad bandwidth " Limited number of layers N<10 layers required for 200 as pulse (@13nm)

Narrow bandwidth coatings for picking a single harmonic Higher order of multilayer mirror: 2dsin" = m# ( m= 2,3, ) Isolate a single harmonic order FWHM = 1.8 ev Reflectivity 0.6 0.5 0.4 0.3 0.2 0.1 0 (2% relative bandwidth vs 3.5% for typical coating) 85 87 89 91 93 95 97 Photon Energy (ev) Reflectivity 0.5 0.45 0.4 0.35 0.3 0.25 0.2 0.15 0.1 0.05 0 2.5 ev 1.2 ev narrowband typical 25 26 27 28 29 30 31 Photon Energy (ev)

Aperiodic supermirror with 20 ev bandwidth 0.25 Reflectivity 0.20 0.15 0.10 0.05 Measured Simulated 0 120 130 140 150 160 170 Wavelength (Å) A. L. Aquila, F. Salmassi, F. Dollar, Y. Liu, and E. Gullikson, "Developments in realistic design for aperiodic Mo/Si multilayer mirrors," Opt. Express 14, 10073-10078 (2006)

Intrinsic HHG chirp Chirp in sub-fs scale: Different energy photons are emitted at slightly different times 1 τ = 558 as Ε = 59 ev Distance from Ion (nm) 0-1 47 ev 69 ev 94 ev 106 ev λ = 800 nm I = 5 x 10 14 W/cm 2 Neon (I p = 21.6 ev) -2-90 0 90 180 270 360 Time (Phase of E-Field)

Chirped Mirror for Phase Control Effective depth for different wavelengths are different Aperodic mirror would provide more control of the spectral phase across wide bandwidth

Chirped multilayer mirrors with controlled phase can be used to compensate chirp for pulse compression Reflectivity 0.8 0.7 0.6 0.5 0.4 0.3 standard M.L. Aperodic M.L. with positive chirp Reflectivity Mo/Si Aperodic M.L. with negative chirp Phase (rad,) 40 35 30 25 20 15 negative chirp Reflected phase positive chirp Mo/Si Quadratic phase associated with a linear chirp 0.2 10 0.1 0 75 80 85 90 95 100 105 Photon Energy (ev) 5 standard M.L. (no chirp) 0 75 80 85 90 95 100 105 Photon Energy (ev) A. Aquila et al, Opt. Lett. 33 (455), 2008

References F. Krausz, M. Ivanov, Review of Modern Physics 81, 163 (2009). P. H. Bucksbaum, Science 317, 766 (2007) E. Goulielmakis, et al., Science 317, 769 (2007) H. Kapteyn, et al., Science 317, 775 (2007) K. Kulander, K. Schafer and J. Krause, in Super Intense Laser-Atom Physics, NATO Advanced Study Institutes, Ser. B, Vol. 316 (Plenum Press, New York, 1993). P. B. Corkum, Phys. Rev. Lett. 71, 1994 (1993). M. Lewenstein et al., Phys. Rev. A 49, 2117 (1994). C. Lyngå et al., Phys. Rev. A 60, 4823 (1999). P. Salières, A. L Huillier and M. Lewenstein, Phys. Rev. Lett. 74, 3776 (1995) A. Rundquist et al., Science 280, 1412 (1998). M. Drescher, et al., Science 291, 1923 (2001). M. Hentschel et al., Nature 414, 509 (2001). R. A. Bartels, et al., Science 297, 376 (2002) R. A. Bartels et al., Opt. Lett. 27, 707 (2002). A. Baltuska, et al., Nature 421, 611 (2003). A. Paul et al., Nature 421, 51 (2003). E. Goulielmakis, et al. Science 305, 1267 (2004). A. L. Aquila, et al., Opt. Express 14, 10073-10078 (2006) E. A. Gibson et al., Science 302, 95 (2003). S. X. Hu and L. A. Collins, PRL 96, 073004 (2006). X. Zhang, et al., Nat. Phys. 3, 270 (2007). O. Cohen, et al., Phys. Rev. Lett. 99, 53902 (2007). A. L. Cavalieri, et al., Nature 449, 1029 (2007) G. Genoud, et al., Appl. Phys. B 90, 533-538 (2008). A. Aquila et al, Opt. Lett. 33 (455), 2008. Tenio Popmintchev, et al., Opt. Lett. 33, 2128 (2008) Jong Ju Park, et al., Opt. Lett. 34, 235-237 (2009)