‘US 2015006: cu») United States cz) Patent Application Publication Popmintchey et al. (64) GENERATION OF VUY, EUV, AND X-RAY LIGHT USING VUV-UV-VIS LASERS oy V. Popmintchey, Boulder, CO nintche, Boulder, Tenlo V. Popmintehev, Boulder, CO (US); Dimitar V. Popmintehey, Boulder, Co (US); Margaret M. Murnane, Boulder, CO (U Boulder, CO (US) Henry C. Kupteyn, (21) Appl. Nos M77. 883 (22) Filed Sep. 4, 2014 Related US. Application Data (©) Provisional applica 4.2013, jon No. 61/873,794, filed on Sep. ao) Pub. No.: US 2015/0063385 Al (43) Pub, Date Mar. 5, 2015 85AL ication Classification GI) Ince. HOIS 3/109 HOIS 3/108 (200501) (006.01), (2) U. oe HOLS 3/109 (2013.01); HOTS 37104 (201301) usec 372 on ABSTRACT A metho for extending and enfsancing bright coherent high ‘order harmonie generation into the VUV-EUV-X-ray regions ‘of the spectrum involves a way of accomplishing. phase ‘matching or effective pose matching af extreme upoonver sion of laser light at high conversion efficiency. approaching 10" in some spectral regions, and at significantly higher photon enenies in a wavepuide geometry, in a self-guiding oometry 2 gas cell, of a losely focusing geometry, contain. ing nonlineae medium, The extension nl enhancement ofthe coherent VUV, UY, X-ray emission to high photon energies relies on using VUV-UV-VIS lasers of shorter wavelength This leads 4 enhancement of macroscopic phase matching parameters due to stronger contribution of linear sd noaline ar dispersion of both atoms and ions, combined witha strongPatent Application Publication Mar. 5, 2015 Sheet 1 of 25 US 2015/0063385 Al 106 4 i186) Figure 1A Figure 1BPatent Application Publication Mar. 5, 2015 Sheet 2 0f25 US 2015/0063385 Al Laser Propagation Geometry Guided beam geometry i) Keep - <— <> Zraviich medium Figure 2A Loose-focus geometry QS T F —_——_—> = Zrayleigh t Figure 2B -medium®* ZRayleigh Laser beam self-confining in space and time = Ge F< >_> Zrayich —— Lmedium Figure 2CPatent Application Publication Mar. 5, 2015 Sheet 3 of 25 US 2015/0063385 Al Figure 3A Laser Laser , (low divergence) Figure 3C Figure 3D HHG Intensity HHG Intensity Figure 3EPatent Application Publication Mar. 5, 2015 Sheet 4 of 25 US 2015/0063385 Al Optimized driving laser phase velocity (optimized index of refraction) /NEWREGIME IIA NEWREGIMEIIIB\\ / OLD REGIME II ATOMS + ATOMS + LOW-CHARGED MULTIPLY-CHARGED ATOMS IONS (ONS Na ' ' 1 Muo= C Mui t Ul t Vasa=¢ > Vaasa” € » Vussca® C N \ TAN Figure 4A Figure 4B Figure 4C (Prior Art) Resulting laser group velocity NEW REGIME II A NEW REGIME IIIB \ / OLD REGIME II {ATOMS + ATOMS + LOW-CHARGED MULTIPLY-CHARGED ‘ATOMS IONS IONS 1 1 Mee Vine = SHE NY 1 “4 Musser = 7 VuseasC > | ai { ' N\ 7. , Figure 5A Figure 5B Figure 5C (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet Sof 25 US 2015/0063385 Al Optimizing driving laser phase velocity NEW REGIME Ill A ATOMS + LOW-CHARGED IONS (HIGH LASER INTENSITY RANGE) Figure 6A NEW REGIME III B ATOMS + MULTIPLY-CHARGED IONS Ming ® 1 (VERY HIGH LASER INTENSITY RANGE) AY, | Figure 6C (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet 6 of 25 US 2015/0063385 Al Spectral domain (Old Regime II) OLD REGIME | OLD REGIME I! Laser Spectra HHG Spectra OLD REGIME! 1Oonm 1nm O.1nme1A 1ev 10ev 100 ev kev 10 keV Log Photon Energy Figure 7A (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet 7 of 25 US 2015/0063385 Al Spectral domain (New Regime II] A and B) OLD REGIME | NEW REGIME Ill A and B Laser Spectra HHG Spectra go ‘OLD REGIME | ——_> a) Tena eee) ie Log Wavelength 1200 nm 10nm anm O.lnm=1A Hard Xrays ev 10 eV 100 ev kev 10 kev Log Photon Energy Figure 7BPatent Application Publication Mar. 5, 2015 Sheet 8 of 25 US 2015/0063385 Al Spectral Shape (New Regime III A and B vs Old Regime I!) HHG Spectra SUPERCONTINUUM OLD REGIME II DISCRETE NARROW-BAND HARMONICS ISOLATED NARROW-BAND HARMONIC NEW REGIME Ill A and Bi i SUPERCONTINUUM ' Log Wavelength 10nm ai 100 ev Log Photon Energy Figure 8Patent Application Publication Mar. 5, 2015. Sheet 9 of 25 Macroscopic HHG Flux (Old Regime |, same laser wavelength) US 2015/0063385 AI LOW LASER HIGH LASER INTENSITY INTENSITY ‘ ‘ ' a 1 Macroscopic HHG flux pase 7 7 1 Log Wavelength 8 ony nm o1nm=th 100 Amy T T | Caw T _Soft X-rays ov] ev ew] 100ev Log Photon Energy Hard oerays kev 10 kev Figure 9A (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet 10 of 25. US 2015/0063385 Al Macroscopic HHG Flux (Old Regime Il, increasing laser wavelength) SHORT LASER LONGER LASER WAVELENGTH WAVELENGTH 7" MID-IR i i = 0 Phase-matched macroscopic HHG flux Log Wavelength i 100m ¥ 10am mm OAnm=14 Qe ---- eee ee 1 fl i 1 1 1 i Hl 1 Hl 1 i 1 1 1 i 1 1 1 i 4 Lev toe 100 ev kev TO kev Log Photon Energy Figure 9B (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet 11 of 25 US 2015/0063385 Al Macroscopic HHG Flux (New Regime III, decreasing laser wavelength) SHORT LASER SHORTER LASER WAVELENGTH WAVELENGTH NEAR-IR \VIS-UV-VUV | Effectively) Phase-matched Imacroscopic HHG flux i 1 Log Wavelength ' ¥ 100nm¥ 10pm mm OtnmeiA TT T T y IR vuv’ ‘Soft rays Vi —— ui EUV) Hard X-rays. 1 1 . r eV 10ev 100ev kev 10 keV) Log Photon Energy Figure 9CPatent Application Publication Mar. 5, 2015 Sheet 12 of 25 US 2015/0063385 Al Pulse Durations (Old Regime II vs I) OLD REGIME | OLD REGIME II Laser pulse HHG pulse duration duration 1 picosecond 1 femtosecond Lattosecond Lzeptosecond Log Time Figure 10A (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet 13 of 25. US 2015/0063385 Al Pulse Durations (New Regime III A and B vs Old Regime |) OLD REGIME! NEW REGIME III A and B Laser pulse HHG pulse duration duration Lpicasecond femtosecond 1 attosecond 1 zeptosecond Log Time Figure 10BPatent Application Publication Mar. 5, 2015 Sheet 14 of 25. US 2015/0063385 Al Pulse Shapes (Old Regime I!) Figure 11B (Prior Art) Driving Laser Pulse Tusen Taser swan Figure 11A t : Tuan aee (Prior Art) LASER macro oe X-ray Pulses Tyasee/2 Toray FWHM . Figure 11C (Prior Art) Tray FWHM Figure 11D (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet 1S of 25 US 2015/0063385 Al Pulse Shapes (New Regime III) Figure 12B Driving Laser Pulses Teaser Taser FWHM Figure 12A X-ray pulses i Figure 12C Teeay FON Figure 12D Tray FinaPatent Application Publication Mar. 5, 2015 Sheet 16 of 25 US 2015/0063385 Al HHG Pulse Durations (New Regime III A and III B vs. Old Regime I!) Tretorn Leo HG Puse Duratons a jp —f ff Figure 13Patent Application Publication Mar. 5, 2015 Sheet 17 of 25 US 2015/0063385 Al UUpeonvertes Photon Energy keV] Efficient HHG (New Regime III A and B vs Old Regime I!) 50; Hard X-rays Soft Xrays TiSapphire Figure 14Patent Application Publication Mar. 5, 2015 Sheet 18 of 25. US 2015/0063385 Al Efficient UV-Driven HHG (New Regime III B) ATOMS + MULTIPLY-CHARGED IONS (VERY HIGH LASER INTENSITY RANGE) XRAY HH FROM MULTIPLYAONIZED ARGON. eer g, | I | = g K A | | I \ ’ 2 tp i 2 oo eo PHOTON ENERGY, iM Figure 15A HHG INTENSITY finger scale) AMI AU Ms 200 PHOTON ENERGY [eV] ae * Arte > Aree Figure 15BPatent Application Publication Mar. 5, 2015 Sheet 19 of 25. US 2015/0063385 Al Efficient UV-Driven HHG (New Regime III A) ATOMS + LOW-CHARGED IONS {HIGH LASER INTENSITY RANGE) 4 3 He i Bo 2 : | oan Wha Too 3089 380 a00 a0 Photon Enory (ho E E E B & : 5 z Q S 3 o 7 0 ui a a 7 Figure16Patent Application Publication Mar. 5, 2015 Sheet 20of25 US 2015/0063385 Al Critical ionization (New Regime III A) 500 = Ar = = ‘\ 2 \\ With spatial Z 900 \ veraeng e . < \ aoe : 9° \ = Without spatial \ % 100} averaging XY E a © % Gs O4 08 08 1 LASER WAVELENGTH [y m] Figure 17Patent Application Publication Mar. 5, 2015 Sheet 21 of 25. US 2015/0063385 Al Efficient UV-Driven HHG (New Regime III A) ATOMS + LOW-CHARGED IONS. (HIGH LASER INTENSITY RANGE) Theoretical Phase Matched Yield Theoretical Single-Atom Yield - TDSE 5 He 02 03 04 05 06 07 08 Laser Wavelength um] Figure 18A 3 aS = § 00) i £28 400) 0274 see | 252 200 Epa eel Les | Ar 5 Zo Be 5x10) a 0.4 - 5 oo “9.7 08 3 0.10 95 08 .05 ~~ 9.4 0 Photon Energy [keV] 0 03 fen verona Figure 18BPatent Application Publication Mar. 5, 2015 Sheet 22 of 25 US 2015/0063385 Al Isolated Harmonics (New Regime III A and B) = 0.27 um e ~96.4 eV 2a ~ 250 p= 3 ino | 2°) 43 nm HHG BEAM RhsBe+Si filters | a a a a a nD PHOTON ENERGY [eV] Figure 19A i ~96.4 eV ~105.6 el po 2M 250 Eo | = 1000) | 2 Rh+Be filters | || ae oe ee PHOTON ENERGY fe) Figure 19B xo! a 7 q | | ev E'} | naan 300 ey | & 2 | | sn fitter a a a PHOTON ENERGY [eV] Figure 19CPatent Application Publication Mar. 5, 2015 Sheet 23 of 25. US 2015/0063385 Al Phase Matching Temporal Window New Regime III A and B 24 = 0.27 wm Large number of laser cycles of ‘Ak(plasma)/Ak(atomesions wont Time [femtosecond] Figure 20A Old Regime | ‘Akiplasma)/Ak(atomssions) oxy Time [femtosecond] Figure 20B (Prior Art)Patent Application Publication Mar. 5, 2015 Sheet 24 of 25. US 2015/0063385 Al Nonlinear medium Total index of refraction of atoms ‘Total index of refraction of ions (hy Lutime) 208 210 toose- focusing geometry Beam selt- ‘confining Imspace and 212 Waveguiding geometry Max flux at desired Pays Figure 21Patent Application Publication Mar. 5, 2015 Sheet 25 of 25 US 2015/0063385 Al Optimization of UV-Driven HHG (New Regime III B) Darsen=0.27 wm 400 350) OF 300) e £250) @ 3 200) E 160) +100) | fl 50) ! Es) 100 150 200 250 300 PHOTON ENERGY [eV] Figure 22US 2015/0063385 Al GENERATION OF VUY, EUY, AND X-RAY LIGHT USING VUV-UV-VIS LASERS [0001] U.S, Pat. App. No, 61873,794, fled 4 Sep, 2013, is ‘ncomporated herein by reference. U.S. Pat. No. 6,151,155, filed 29 Jul, 1998 and issued 21 Nov. 2000 is incomporated herein by reference. US, Pat, No. 8462,824 filed 22 Apr. 2010 and issued 11 Jun. 2013 is incorporated herein by r= BACKGROUND OF THE INVENTION 0002] 1 Field ofthe Invention [0003] The present invention relates to extending and ‘enhaoeing bright colterent high-order hamonie generation Jno the VUV-EUV-X-ray regions of te spectrum. Inparicu- Jar, the present invention relates to phase matched and effee- tively phase matched generation of VUV, FUV, and X-ray Fight using VUV-UV-VIS laser pulses. 10008) 2. Discussion of Related Art [0005] This inveation is related to thre previously deme strated techniques, implemented in # novel regime of para ‘eters that contrasts with the parameters of all techniques, ‘demonstrated to date: 0006] The frst related technique is developed by some of the inventors inthe current application ad includes method and device for phase matching the generation of high har- ‘monic radiation in a waveguide, which is patented (U.S, Pat No. 6,151,155, incorporated herein by eference) Using this technique and, typically, a Ti:Sapphire laser of a wavelength ‘of 08 jum to drive the high humonic process, full phase matching ofthe process can extend to FUVesoft x-ray wave- Jengths of about 10m, Therefore, in practice the cup Thx produced is significant enough to enable applications using Jight with wavelength no shorter than 10 am. In this scheme, the generation of soft x-rays of shorter wavelenaths requires ‘an increase in driving laser intensity. However, sealing of macroscopic parameters (see typical values in Table 1, Regime D does notallow forextending the phase matching of the process to shorter x-ay wavelengths, at the same time. Higher intensities result in too much ionization of he pas, ‘degrading the phase matching conditions and limiting both the fux and the coherence ofthe generated lixht. Emission at wavelengths shorter than ~10 nm can be observed but it ‘originates from a region of the nonlinear medium of short, length, and.or with a low density of emitters, and in the presence of lange number of fee electrons AIT hese fictors ‘Sramatically decreasing the x-ray flux to levels nat wsefil for applications, Typically the emission originates from a shor ‘coherence length of <1-100 jim and both atoms and ions can ntharmonies of very high photon energies. However, due to the very short coherence length—that ean be much shorter than the medium absorption length and medium length the ‘emission from ions in the high photon energy range is 3-4 ‘onders of magnitude lower than the emission from atoms Timited only within the low photon energy range. [0007] The second technique rested to this invention isthe dea that a longer-wavelength civing laser can be used 0 tenerate X-rays of shorter wavelength. This idea exginates from the simple theoretical model that well describes the high-order harmonic generation process. (Kuander; Cor kum). However, subsequent theory predicted that using longer laser wavelengths 2... 1 generate shorter X-ray ‘wavelengths comes ata cost o's significantly lower single ‘atom yield (Le. the amount of Xray ht generated for each, Mar. 5, 2015 ‘tom in the nonlinear medium, predicted 10 Seales 2. 2). Initial attempts fo generate shorter-wavelengily X-rays using laser wavelengths as long as 1.5 um (Shan, PRA 65, (011804 2001) supported this prediction of diminishing lux ‘This and later experiments were done ina gas jet goometry using macroscopic parameter regime similar to the well ‘known Regime I (low gas pressure (on the order of tens 10 Jhundreds of toe) inthe interaction region, anda shor propa sation length (onthe oder of.1-1 mm)),and didnot observe ‘ux that would make their approach usable as a general purpose coherent X-ray source. Furthermore, more recent {quantum ealeuations suggested that the single-atom yield drops even more dramatically with laser wavelengths and scales 88 Fra? The ideas in this approach imply that shorter-wavelcagth lasers may give rset significantly bright ‘emission froma single emitter limited to the long-wavelength HG range, however, the macroseopie optimization of the HHG upconversion has not ben considered neither for shorterwavelength nor for longer-vavelengt lasers [0008] To remedy the low conversion effiiency observed inthe above-mentioned work, in past work we developed a third tehnique—a method for optimization of phase matched conversion of mid-infrared laser light into the X-ray regionof the spectrum. By using high-pressure medium and a foose- Toeusing geometry. This approach, devised by many of the same inventors a8 the current inveation, is described is described in Popmintehev et al, US. Pat. No, 862,824 (ncorporated herein by reference). In contrast with the pre- viously discussed scheme in Regime I, the inventors demon- strated that both the X-ray radiation from a single atom, as well as phase matched conversion of this process, can be extended to the generation of much shorter wavelengths. la order to produce significant X-ray ux, this techniques requires a regime of parameters (see optimal parameters in ‘Table 1, Regime ID), contrasting withthe parameters in the scheme ilstrated in Regime lusing Te:Sapphire lasers. This phase matching sealing to shorter wavelengths is achieved throvgh increasing. the laser wavelength while slightly decreasing the laser intensity. Second, a nonlinear medium of ‘much higher density (note the optimal gas pressure of mul- ‘iple atmospheres is required when using longer wavelength lasers to allow the X-ray beam intensity to build o opin conversion efficiency. This technique employs nonlinear ‘media that is only barely ionized, with many neutral atoms still remaining after the generation process teminates. Care- fully designes macroscopic parameters lead to corent build ofthe X-ray signal over extended optimal can bea sigilicanly lng em or longer). The result isa fully spatially and temporally coherent, well directed, X-ray beam, ‘Tunabilty of this broadband X-ray source is achieved by changing the laser wavelength in the IR region and by ehang- ing the intensity and/or the medium, plus adjusting the ‘medium parameters, The tunability range can be from hun- dreds of tm to sub-nm, Helium gas i a good candidate as a ‘nonlinear medium usable for «tunable source over a broad range of X-ray wavelenglhs. Other noble gases can also be sed in some regions ofthe spectrum. Finally, dhe method for ‘optimization in Regime I implies that using shorierswave- length taser ean generate bright phase-matched TH from parlially ionized atoms ia the long-wavelength VUV range. [0009] A need remains in the art for using shorter wave- length driving lasers inthe VUV-LIV-VIS region of the spec- ‘rum to benefit from the strong single-atom yield, whiUS 2015/0063385 Al simultaneously extending this upconversion in an ficient ‘vay well into the shorter wavelength VUV, EUV. and X-ray regions SUMMARY OF THE INVENTION [0010] _Ttisan object ofthe present invention fo use shorter ‘wavelength driving lasers in the VUVGLIV-VIS region ofthe spectrum for phase matched generation and effectively phase matched gencration (defined herein as generation with opti mized phase mismatch) of coberemt VUV, EUV, and X-ray High, {0011} Embodiments extend and enhance bright coherent high-order harmonic generation into the VUV-EUV-X-ray regions of the spectrum. This method involves a previously unrealized, straightforward way of achieving relatively high upconversion of laser light to VUV, EUV, and X-ray light at ‘conversion efficiency that in some eases an approach 10", “This extension of HING relies on using VUV-UV-VIS lasers ‘of shorter wavelength to deve the upconversion process, and ‘employing focused intensities ofthese lasers that cause sab- ‘antialjoization ofthe noalinear medium. We show thatthe tse of short-wavelength driving lasers ina properly designed Toose-foens, waveguide geometty, or laser self-aviding oometry over an extended distance tht i similar of greater than a coherence length ean unexpectedly lead to 3 non obvious, favorible enbuncement of macroscopic phase matching parameters due to stronger contribution of Tineae ‘and nonlinear dispersion ofboth atoms aad multiply charged jons. The resulting strong macroscopic yield of VUV-t0- EUVa0-X-ray photons is combined with the significantly increased microscopic singlestom yield that is inherent t0 driving HIG with shorter wavelength laters, In 3 properly designed and implemented geometry, well-drected, ultrafast VUV-EUV-X-ray beams of full temporal und spatial coher- ‘ence an exhibit a nearly quasi-monochromatic spectrum tat ‘consists of a relatively small number of well-separated har- monies, or a single quasi-monochromatic harmonic. In the time domain, the high harmonic ight ea bea isolated pulse, in of pulses whose separation decreases as we decrease the driving wavelength, or this rain of pulses may even mene intoa single relatively long-duration pulsethat corresponds 0 ‘an isolated single harmonic. The generated harmonies are also semi-continiously tunable throwgh varying the laser ‘wavelength and/or changing the nonlinear medium. [0012] | Fmbodiments of the present invention use, fis shorter wavelength driving lasers in the VUV-UVVIS region ‘of the spectrum (sce Regime Il in Table 1) in contrat tothe work of US. Pat. No. 8,462,824. Second, simultaneously With decreasing the laser wavelength the present invention significantly increases the laser intensity by few orders of magnitude to the range of 10'-10'* Wiem? or greater. A fundamentally new regime of HIG ean he accessed when laser wavelength, peak power, and focusing geometry are properly optimized. The illumination at tis intensity results Inreltively strong ionization ofthe nonlinear medium, oft creating multiply charged ions (eg. Art, Ar*, Ar, Ae, Ae, ete). Furhermore, using shorter VUV-UV-VIS laser rans thatboth the linear and nonlinear index of reffaction of the neutral atomie and ionie nonlinear medium are signiti- cantly large since thes laser wavelengths approach the UV resonances of atoms Finally, weextend the interaction length ‘withthe nonlinear medium were such high laser intenst are maintained by using oose-foeusing, waveyuiding geo Mar. 5, 2015 ety or laser sel yuiding geometry ta length thats optimal {orellicent HIG upoonversion. [013]. The present invention is generally separated into ‘wo regimes Regime ILA of igh laser intensity where full phase matching balance can be achieved, and Regime TB ‘where there is finite phase mismatch but iis strongly mit ate. RIE DESCRIPTION OP THE DRAWINGS. [W014] FIG. 1. is schematic block diagram illustrating apparatus for phasesmatched and effectively phase-matched high-order harmonic generation (HLIG) in the VUV-EUV-X- ‘ay regions of the spectrum according to the present iven- [0015] FIG. 1Bis schematic block diagram showing inject- ing of a nonlinear medium in the interaction region and ‘optional differential pumping to vacuum, [016] FIG. 2A isa schematic hlock diagram illustrating a uid beam geometry embodiment ofthe present invention. [017] "FIG. 2B is «schematic block diagram illustrating & Joose-focusing geometry embodiment of the present inven- ‘io, 0018} FIG. 2C isa schematic block diagram illustrating 2 Jaserself-guiding geometry embodiment of tepresentinven- [019] FIG. 38 is an isomeric schematic block diagram ilkistating interaction within a waveguide for strong, con- struetve, cohereat build up of HHG light. 0020} FIG. 3B is a side-view schematic block illustrating how output pulse intensity increases and be diverge decreases with phase matching or elfective phase ‘matehing within the medium, [021] FIG. 3C is a side-view schematic block diagram illustrating coherence length within the medium according © the present invention. 0022} FIG. 3D isa plot showing te intensity of the outp pulses with phase matching over the interaction region length comparable to a short absorption length [0023] FIG. 3F isa plot showing the intensity of the output pulses with eifective phase matching over the interaction ‘epion comparable to along absorption length. [024] FIG, 44 is schematic flow diagram sllustating phase velocity matching of the driving laser light and the ‘fenerated lightin Regime IIIA according the present inven- [0025] FIG. 48 is a schematic flow diagram showing the reduced phase velocity mismatch in Regime IIB in the present invention. [0026] FIG. 4C (Prior An) is u schematic Dow diagram showing phase velocity matching with Regime I. [0027] FIG. A is a schematic flow disgram lusting resulting minimal group velocity mismatch of the diving Jaser light andthe generated light in Regime IIIA according to the present invention. [028] FIG. SB is schematic Now diagram illustrating resulting reduced group velocity mismatch in Regime THB fceording tothe present invention, 0029] FIG. 8C (Prior Art) is a schematic ow diagram illustrating resulting strong group velocity mismatch of the vn ihn he generat ght in prorat Regine [0030] FIG. 64 is adetsiled schematic flow diagram illus {rating the phase velocity matching ofthe driving laser light and the penerated light where dispersion of atoms axl of lowsUS 2015/0063385 Al charged ions can compensate large plasma dispersion i Regine ILA acconing othe preeot vention. [0031] FIG. 6B isa detailed! schematic How cgram illo trating he eed hae velocity mismatch where dispersion ‘oF atoms and predominaally dispersion of mulply charged fons can mitigate larger plas dispersion in Regine 1B ‘second to the present invention. 0032] "FIG. 6C (Prior An) isa detailed schematic flow agri illustrating te pote velocity matching othe driv= fing liner light andthe generated ht in pio at Regine I, where atomie dispersion compensates plasma dispersion and Jonicesperson sneliibe [0033] "1G. 7A (Poe.An) isa schematic spectral domsin agra illustrating the eons ofthe laser apctea aa the Uupeonverted FG spectra with phase matching aeording fo Prior art Regimes and [0034] FIG. 7B is a schematic spect domain dinar ‘stating the regions ofthe laser Specea and the efit Upeonverted TG spectra according to present invention Regimes ILA and 1. [0035] FG. Bis aschematic spectral domain ngram ills trating ost pole spectral shape of upconverted IHG ight ‘ovonting (0 prorat Regime Il and the preset iention, Regimes ILA and II. 10036) FIG.9A (Prior Anis. schematic diagram il ing thecontol parameters, optimizing parameters, ode ne macroscopic HHG fi in conventional ir poe at Regine Land shows parneers and resus varios wane Jeng 10037] _F1G.98 (Prior An) isa schematic diggram illus ‘ng the cone parameters, optimizing parameters an eel jng macroscopic HIG fax in conventional for poe at Reine I and shows parameters and resist varots wave- Jengths. 10038) FIG. 9Cis schemati diagram illostating the con- trol parameters, optimizing parameters and resulting moe scopic HG fx Regime Ill sconting to the presen inven- 10039] FG, 104 (Prior An) isa sehematic ime donsin agri illustrating the regions of the driving laser pulse ‘rations and the HHG pulse durations with phase matehing Sn prior art Regimes I and Il st yarious wavelengths. [0040] "FIG. 108 isa schematic ime domain ligaramills trating the regions ofthe driving laser pose durations andthe HG pulse durations with phase matchinginprioean Regime [and in phase matching and effective phase matching in Regime III aecorting 10 the present invention at various ‘wavelengths. [0041] FIGS. 118-D aretime donsin diagrams using input laser pulse shapes and output HHG pulse shapes ssvonding to prior art Regime I 10042] FIGS. 124-D azetime domssin diggrams isting fnput laser pulse shapes and output HHG pulse shapes ‘according Regine IT ofthe cuerent ivention 10043] FIG. 13 isa time domain diagram presenting the senerted, chirped, HEG pulse dations andthe enim HG pulse durationsifthe pulses ae compressed for prior art Regt Ifand Regimes ILA and I aeconing tothe present invention at varios wavelengths {0048} FIG, 14s plot of HEC phase matching Kimi foe Prior art Regime Il ad ecient HAG upeonversion photon ‘cergis in Regimes ITA and IIIB according tothe resent invention [0045] "FG, 154 is a plot shossing example experimental data demosstrating specially selected right diseretehar= Mar. 5, 2015 monic i the X-ray seaion ofthe specu up tothe water ‘window ia Regime IIB according tothe present ivention, [0046] FIG. 188 isa plot showing example experimestal data presenting bright dseretearmoniesspaning the VUV- FUVXray spectal regions and comesponding. multiply clurged eaters [0047] FIG. 16isa por showing examploexperimenta data lmonstating wlteright discrete armonis inthe EUN Spectral regioninRegimelIIA accoing othe pesentaven- {0048} FIG. 17s plot showingan example estelation of the etc ionization level of a gs versus laser wavelength {orRegime IIA according the presen invention, with nd without spatial averaging. [0049] FIG. 184 isa pot showing an example calculation ff the expected HIG easission from a single atom versts diving laser wavelength for Regime IIIA according t0 the present ination {0080} "FIG. 188 isa plot showing an example calculation ofthe expected elicea macroscopic harmon inteosly ver sus conesponding HG photon energy snd driving laser ‘wavelenah for Regime IIIS according the pesca ven [0051] FIG. 194 isa plo showing example experimental data demonstrating beam profile and» bright narrow-band EUV harmonic around 13 nm isolated by a eombition of Jow-pass and high pas thin il filters and by using specific dese intensity. {0082} "FIG. 198 is plot showing example experimental data of to bright narrow-band EUV harmonies ound 13 ated bya combination of low-pass ad high pass hin {im fiters and by vsing a specif laser intensity. {0053} FIG. 19C isa plot showing example experimental a bright aerow-band VUV haeronics0- lelow-pans ad high pas thi fi itera by sng a speclc ser intensity: [0084] FIG, 204 is a pot showing an example of an extended temporal window of efficient upconversion over a large number f diving laser yes for Regime I scoring tothe present invention. {0085} _F1G.20B Prior An)isa plot showing anexampleot 4 narrows temporal window ef upcomersion for rie art Regine (0086) FIG. 21 is flow diagram isting tps in she proces of global optimization of HAG with phase matching Seciective phase matching according tothe preset saven= tion, and tps in sslectng the opis parameters foe most cient HG ata desied HETG wavelength. [0057] F1G.2isaplotshowing exsmpleexperinental data monsteing presse optimization of Uvedrven HEC spnning the FUVAVUV-X-ray regions of the spectrum for ‘epime IIB according tothe present invention. DETAILED DESCRIPTION OF THE INVENTION [0058] Prior to this invention t was widely accepted that [phase matching in extreme frequency upconversion in highly Jonized plasma couldn't be obtained due to the fact that free clectron dispersion dominates the process and no Tonger is balanced by the neutral atom dispersion, Here, we demon- strate that it i possible to achieve such balance o stongly mitigate the phase mismatch. Using. shorter wavelength VUV-UV-VIS lasers to drive the HHG process means that both the linear and noliscarindex of refraction of te neutral atomic nonlinear medium are significant since these laser lenas approach the UV resonances of atoms. AS &US 2015/0063385 Al result, the optimal laser intensity i significantly higher whieh Jlurther increases the nonlinear dispersion contribution whith Jncreases wth laser intensity ~n,0""""1, me). Nex, Hinear 1nd nonlinear indices of refraction of ions can be nearly as large as those of neutral stom, and will increase as we use shorter driving later wavelengths. Furthermore, since highly ‘charged ion are created later inthe ler pulse when the laser Intensity is higher, the nonlinear dispersion term can be aso Significant because oF the higher laser intensity =n,°°" "I, (Gime), Thus there is significant dispersion contribution both from neutral atoms and ions. Ths s balanced against a free ‘electron dispersion term of opposite sign, and of greatly ‘diminished magnitude compared with its value at longer jnfred savelengths, Purthermore, the coherence length of the upconversion process to fist upproximation (assuming dominant plasma dispersion) scales approximately as Lo l/(Q" in) Wiha} being the armonic order, and whieh fora given X-ray enemy is smaller ifa shorter-wavelength diver is used. Combined, these macroscopic propagation “actors allow for significant coherent signal buildup for X-ray HG even inthe ease of very high laser intensity resulting in very high limiting ionization levels that in some cases can be S106. 10089] When the length of the nonlinear medium, the absomption depth ofthe medium tothe generated X-rays, and (wen Deny Mar. 5, 2015 the coherence length all reach comparable valves, HG ipeonversion js elfectively phase matehed, Both these scal- ‘ng considerations as well ax experimental data suggest that ‘optimization of the interaction geometry can approach this {dealin the ease of short-wavelength driving lasers, and very high intensity and comesponding very high photon energies. [0060] Furthermore, as mentioned previously the X-ray ‘emission yield per atom also increases strongly with the use fof shorter drive laser wavelengths. This reslts in shorter ‘excursion distance ofthe rescattering electron, Due to loser {quantum difluson, the recombination probability is signif cantly increased, with yield from a single stom that scales Songer than ~)eaqc*» TDSE caleulations show that th ‘ingle-atom yield tier phase matched illumination sales hea oF ven Faster since much higher laser intensities compared to Regime I are allowed. Thus, regardless of hav= ing a finite coherence length the conversion efficiency can be Significantly high compared to the peor art. {0061} Table 1 shows comparison of practical parameters when scaling the HHG process towards generiting shorter X-ray wavelengths, using near-[R O.S mm driving laser (Re- ‘ime prior art) longer-wavelength mid-IR driving lasers (Regime I—prior aft), and shorter-wavelength VUV-UV- ‘VIS lasers (Regime IIT presen invention) TABLE L Regie I psent egine pra) Regine ora) aveton) (oops (lactate) (phrerached ‘ith eg time edna Seeiiupty fer, OIE TOM em om, ccs ie Thy sied or 007% Tigh nia a ed EStencnliy, Nomen Tigi chet om ‘ona on, Range faction angst m+ Range acon of meson mmpler, —— amemperet Siti methon athe solide nonlinear inn ofa mnie inden ‘sowieng——Seurfaomcricn, eu som Se atm Let Nolte Deentesiom Infant see oan Medium Lent mmsatenm, = cao. oath Denetyatte | Imane dom, Conan —10! ae oe Comers Leen Wee Ww 00US 2015/0063385 Al TABLE Regime por an) -continved Mar. 5, 2015 Regine ries) toe) (oo pa (pharemached) (pave ated) Tinos (shy (iil) Finsowiching —Plsmedapenion Newnan Lage muta > 10°7 to S>10" em, This results in a useful nonlinear medium Fength Un gyy, of centimeters to sub 10-100 um. The phase- matched addition of the TING fields means that fax does not vary strongly with wavelength, 10063) |The laser source 102 ener, wavelength, and pulse 104 duration areselocted to maintain phase matched or eflee- vely phase matched HEG 196 generation, Driving source 102 may produce ultrashort driving pulses et any repetition rate or long “macroscopic” plses at any repetition rate with ‘multiple driving pulses under the envelope 10065] | Medium 130 or 132 might comprise atomie gases (for example, noble gases: helium, neoa, argon, krypton. ‘eno, ete.) and mixtures, of molecular gases (for example (lor example ar, et.) Gas mixing apparanis 134s optional In mixtures, phase matching and eflective phase matching relies on the presence ofa target that is lest a nom-ionized compared tothe other species targets fora given peak laser intensity. Therefore, a mixture of targets with diflerention- ination potentials may be desirable. Mixtures allow theless ‘nized medium to contribute to the neutral and inte index oF refraction, Therefore, higher laser intensity canbe employes As a result higher photon energies may be phase matched or effectively phase matched with further increase ia HHG fox. Since the short wavelength driving laser can penetrate higher ‘density plasm, the nonlinear medium may be liguid, of mix- treo lguids,or for example olid state He, Ne ete such that atthemaximum ionization level the eiical plasma deasity at the driving laser wavelength is not exceeded (lor example ‘0% ofthe critical plasma density is reached ata mean charge Z>1 for HO and 0.16 pm laser, 67% of the ertcal plasma ‘density is reached atamean charge Z=I for S10. and0.16 um laser; 59% of the critical plasma density is reached at a mean charge Z=1 for solid H and 0.16 wm laser), [0066] Other optional eatures include a front mirror 122 Torbeam storing a the input to mopitor eam diameter at the entrance of waveguide or gas cell 120, Laser bear 136 is ‘eoupled into monitoring equipment 138 in order to optimize ‘waveguide mode coupling, to monitor and eontrol beam pointing, as well as to monitor the laser pesk intensity on {arget. Monitoring 138 may also monitor the input spectrum. Front miror 122 may be removable [0067] Optional back mirror 112 selects beam 114 for ‘monitoring equipment 116. Monitoring equipment 116 may mage the beam diameter tthe output or at certain propa tion distance, may monitar and eantro! beam pointing. my ‘monitor the beam intensity at the output, and/or may monitor ‘the iaput laser spectrum. Front mirror 112 may be removable ‘orhave a hole for transmission, {0068} "Optional differential pumping 142, 44 orseveral of | them may be provided. input and output of waveguide or gasUS 2015/0063385 Al ell 120, a8 illustrated ia FIG. 1B. ‘diameter tubing is provided along the axis ofthe HG propogation, and the bing restricts the gas ow foran ‘embodiment where the nonlinear medium is ina ges phase, While allowing the driving ser and the generated light through. The gas flow resistance increases significantly with ‘decreases inthe diameter of the tubing and scales as ~D*, whore D is the diameter. The gas flow coming out of the region containing the nonlinear medium ean preferentially be redirected towards bigger diameter region of low resistance pumped by vacuum pumps and can be also additionally steered in this direction by inlined surfiees (e.g 45 degrees inthe example drawing). 10069] FIG. 24 isa schematic block diggram ilusteating @ ded beam geometry embodiment ofthe present invention. ‘This embodiment comprises a hollow waveguide (eyindeical or tapered) filed with @ nonlinear medium. The laser beam 104 is focused to an optimal beam diameter relative to a selected waveguide diameter to couple to a desired ‘waveguide mode orto minimize attenuation losses. The idea js to extend the region of high laser intensity, ic. the Rayleigh age Zgyngi fOWards multiple Rayleigh ranges. Ths sofa significant importance to decrease the techincal challenges with respect to the required laser technology having in mind that the optimal high ser intensities in some cases excoeds >10'*-10"" Wem", Also, this geometry can provide near plane wave propagation of the Taser beam. Such uniform ‘conditions may’ allow for a better collinear (effectively) pPhase-matched upconversion. The waveguide ean also pro- Vide means to contain a gas with uniform pressure Over extended distances and can also provide pressurc-length products that are uniform or with predesigned! gradients that ‘re better controlled compared to gus direly injected into 1 vacuum chamber [0070] FIG. 22 is a schematic block diagram ilustrating 2 Joose-focusing geometry embodiment of the present inven- tion, na loose-focus geometry the medium length can be nich shorter than the region of high laser intensity the Ray leigh range Zengt- Ths, te interaction region is almost in ‘near plane Wave propagation similar to propagation in 3 ‘waveguide, The roguired optimal laser energy can be sig cantly larger, {0071} _FIG.2€ is aschemati block diagram ilustrating @ laser self-puiding geometry embodiment of the present inven- tion. A waveguiding geometry may also assist the formation ‘of self-guided propagation ofthe laser beam. The laser beam. ‘ean collapse to smaller diameter than that atthe entrance of the waveguide and can propagate steadily afer a certain dis- lance, of can propagate a the same diameter regardless of plasma-induced defocusing, This is due toa balance between Kerr lens self-foeusing an plasma-induced defocusing spe- fe fora waveguide structure (je. different from a conven= tional filamentaion effect in tise space) and may coincide ‘with a regime of nonlineae medium parameters and laser pulse parameters that are also optimal for ellcient HG Uupeouversion. Such selF- guiding in space, a stable propaga- tion in space, may be also accompanied by a stable propaga- tion of the laser pulse in time withont aay’ change in pulse ‘duration or with a compression in pulse durtion along the Jimeraction distance [0072] FIGS. 3A-3D are schem: how the optimized VUV-EUV- fe diagrams illstrating ray intensity increases Mar. 5, 2015 Within the medium, as well as the parameters of the HG scheme tht depend on the driving laser wavelength and the HHG wavelength, [0073] FIG. 34 is an isometric schematic block diagram illustrating interaction within a waveguide for a. phase ‘matched and effectively phase matched buildup of high-har- ‘ionic signal, FIG, 3A also shows the phase velocity and the resulting group velocity of the driving laser pulse associated ‘with the propagation of the eazrie Wave and its eavelope, respoctively In an ideal case, the phase velocities oft rivng Tight and the generated Tight has to be matched while the grup velocity mismatch has to be mitigated FIG. 3A also shows interactions within the medium ia the wavewuide, ‘wherein the harmonic fields are generated, and are added construtvely over a finite interaction length [0074] FIG. 3B is a side-view schematic block diagram illustrating how output pulse tensity increases and the HEIG ‘beam divergence decreases with (effective) phase matching Within the medium. The driving pulse phase velocity is ‘matched 1 the phase velocity ofthe generated HAG or the ‘nismateh s greatly minimized. Thus, the cobereaceFength of the (effective) phase matching isextended beyond the optimal snediuss leg Lyin FIG. 3C (deal Ly forsome conditions, or Ly ean be finite) in other words, the entre interaction region fs now equivalent to a (+) region of eon- structive addition of IG fel, [0078] FIG. 3C is a side-wiew schematic block diagram illustrating coherence length within the medium according 0 the present invention. In FIG. 3C constructive addition of HG fields is possible, in contrast to a (-) zone where destructive addition of HHIG fields ean greatly reduce the HG signal. No significant destructive interference occurs. IF there is finite phase mismatch such a selection ofthe eaber- ence length with the respect of the medium length ean be ‘denotedalsoas.an eflectivephasematching Inthe present ar, the coherence length (2, yan) for any HHG wave. Jength can be maintained always relatively long by properly selecting the laser parameters and the nonlinear metim parameters. [0076] Theconerence length ofthe upcoaversion processto Tint approximation scales a8 Lj~I/(Q" pe, assuming very high leet of ionization, andthe relatively Tow harmonic ‘orders correspond to high photon enenies when we use sho ‘wavelength lasers. As a result, this approach allows for si nificantly long eakerence length, that may be comparable to the optimal Jength ofthe medium (ie. close to one or few absorption lengths of the medium), even for high photon ‘energies. Selecting the optimal medium length to be compa rule to the relatively long coherence length ensures strong ccnsinictive buildup of hamonie signal even at very high ionization levelsstrong fre electron dispersion. [0077] FIG. 3D isa plot showing the esulting intensity of | the output HEG pulses over the interaction region. Tt increases strongly with interaction length, until absorption of the generated HING or evolution of the laser pulse inthe pas Timits further buildup of HHG signal. Under phase matehing conditions or greatly reduced phase mismatch, there iscober ent radiation build-up ina very specific direction that redvces the HHG beam divergence, as shown in FIG. 38. [0078] FIG. 34 is a plot showing thot effective phase ‘matching may be achieved also fora inte coherence length that ean be relatively short (eg. 1-500 jum), however, the ‘ium length can be selected to be shorter but comparable ‘Under such conditions a strong coherent buildup ean still beUS 2015/0063385 Al ‘achieved and a desired number of photons can be obtained fice the emission from a single tom significantly increases Jor shorter laser wavelengths. In such an optimization, the ‘absompton medium length may not be raced and absorption Jimited HG upeonversion may not be obtained 10079] FIGS. 4A-6C illustrate phased matched HHG ia three regimes: prior art Regime I, Regime ILA according t© the present invention, and Regime IIIB according to the present invention. Refer back to Table forthe characterises ‘of each Regime. Briefly, in Regime Il, phase matching is ‘achieved a8 balance between neutral tom dispersion and fe electton plasma dispersion that has an opposite sign in 2 Tightly ionized medium. In Regime IIIA, the balance is between the dispersion of neteal atoms in combination with the dispersion of low-chanze ions ofthe same sign, and the plasma dispersion in highly ionized medium, The resulting troup velocity mismatch hereisminimal. la Regime ITB, fll balance cannot be achieved, but the phase mismatch i mi mized by balancing between dispersion of neutral atoms plus ‘utiply-charged ions and plasma dispersion in multiply= ‘charged medium. The resulting group velocity mismatch here ‘increases but it can he relatively small compared to that ia Regime I [0080] FIG. schematic flow diagram illustrating phase velocity matehing of the driving laser light and the _Benerotd light in Regime IILA according tothe present inwen= tion la Regime IILA, phase matching is optimized in a ighly ‘nized mesium, To optimize macroscopie phase matching ia the process of HHG ateans that the driving laser pulse and the generated HHG pulses propagate through the nonlinear ‘medium almost at the same phase velocity. When HHG emis- sion sin the FUV and HIG region ofthe spectrum the HG phase velocity is very close the speed of ight in vacuum Vinegr® and may vary insignificantly when changing the parameters ofthe medium. Therefore, the phase velocity of the driving lasers the ane that has to be primarily optimized through the laser and medium parameters and has tobe also Vz esea*-In principal, while the plasma dispersion speeds up the phase velocity ofthe laser, the normal neutral atom and jonie dispersions slow it dowa, Sings almost all harmonies propagate atthe same phase velocity obtaining phase match- fing ia THING upconversion usually results in simultaneous phase matching forthe whole HEHG bandwidtl, which can be the case in Regimes ILA and B and Regime Il. Not that for HG in the VUV region the deviation from c may be s ‘cantly bigger and the optimal parameters may be modified in ‘compatison to HHG in the EUV and X-ray’ regions. [0081] _InRegimelILA, the indices of reaction (both linear ‘and nonlinear) ofboth atoms andions ineease as we decrease the loser wavelength towards the VIS-UV-VU regions, Fure thermore in this epime the indies of refraction of ions are ‘comparable to that of aoa. 10082} ‘Thus, under some conditions much larger plasma dlispersion can be balanced by neutral atom and ionie disper- sions (Soe FIG. 6A). Ithas boon considered in the past that such a balce i not possible sinve plasma dispersion domi hates the interaction leading toa significant phase mismatch ‘and poor upconversion efficiency. In Regime IA the balance ‘ay'be achieved between neural atom including low charged jonie dispersion and relatively high plasma dispersion. In some instances the neutral atoms may’ be ionized and not present later i the laser pulse. [0083] FIG. 4B is a schems reduced phase velocity mist fe flow diagram showing the teh in Regime TB in the Mar. 5, 2015 present invention. At very high lse intensities in Regi IIB, multiply charged ons can be yourated. Under st conditions fll balance between the phase velocities cannot be achieved, however the phe mismatch is relatively los allowing for effent upconversion Sinee the plasma disper Sion is anger a larger fonizaon levels (due to higher lser Jntensiy), although the tot index of refraction (including Tinea and nonlinear indices) inereses of oth neutral atoms annons the phase velocity ofthe lasers slighty gseter than bt elose © €, vray (oe FIG. 6B) hn Regine IB the eu atoms moy disappear completely quite early during ‘he laser pulsed most ofthe higher order harmonics ye cffcienty generat prodominantly only from ions. n some cases, as many a fe multiply charged ons can counteract the much higher plasma dispersion to greatly reduce the ‘hase mismatch o achieve effective phase matching over a propery selected medium length, {0084} FIG. 4C (Prior An) is schematic flow diagram showing phase velocity matching with Regime Il. Ta prior art Regime Il, phase matching is obained asa balance hetween neutral atom dispersion aad fre electton plasma (se IG. {6(), The balance im Regime Il can be achieved only wp to relatively Jow plasma dispersion since the indies of relae- tion of atoms ad ons decrease and are relatively low as we Jngtease the ser wavelength towards the mil. In this ‘regime, th contribution of any ini isperson is eligible (0085) FIG. 8A is schematic How diagram slhstrating resulting group velocity matching of the dewving laser light and the generated Tight in Regime ITA seeoring to the present invention {0086} - Whilethe pose velocity othe deving laser pels Associated withthe ropaptionof the carrer frequency ofthe levine ld the proup velocity is associated withthe ropa tation of the envelope ofthe eld (refer to FIG. 38)-In Principal, fora medium widh somal dispersion the group ‘locity is altvays smaller than the sposd of ight in vac yon pe ed hl aru Velocity mating eanaot be achioved. Most of the HG light propagstes not ony with iss velciy but aso with group velocity very close 0c area {0087} “Tn Regime 11, the resulting group velocity is ‘hatch under optimal conditions i significantly minimized ‘when he laser wavelength decreased. This means that UV Griving pulse with ethers smaller or @ larger number of cycles can matain phase matching and one can generate ithe a solted HIG burst or a rain of burst wih ilar efcieney per ser eel. In contest fora fe -eyel mid IR ‘ving pulsephose matching con be desiyed orarelatively Small densiyength product and ecient upeonveton ean be precldd. This s hecause the eavelope ofthe lsc eld Jags with respect to the carer field and the amplitide ofthe caries motifed, nce, pase matching is affected. Ths, nls any ditional technigue is used, larger noiber of cles may be desirable fora midlR lsc pase to obtain st0up locity mismatch thats effectively reduced inorderto preserve phase matching. {0088} FIG. 58 is schematic Now digram ilstating resulting reduced group velocity mismatch in Regime IB according othe presen invention. Inthe present invention in Regime IIB, at much higher laser intensities and higher gas pressures compared to Regime IIA, th group velocity mi fateh inerenses. However, since the optiaal propagation [ength can be relatively short the soup velocity walk off effectively smallerUS 2015/0063385 Al 0089] FIG. SC Prive An) i a sehematie Hw diggran ‘losrating resulting group velocity mismatch ofthe deving lnsrfight andthe generated Tigh in prorat Regime I When the phase velocities are mated in the conventional Regine Tas we increase the lser wavelength there is a resting soup velocity mismatch tat i severe. This s due wo igh ‘ptm prssure-length prods eure 10 achieve phase ‘alching and to compensate for ow emission fom a sngle atom. Additonal optimization (eg increasing the number of Insr eyes, pulse shaping, eo techies are need to mitigate the elfoct and preserve phase matching. 10090] FIG. 6A isa detailed schematic fw digram illus testing the phase velocity ntching ofthe driving laser ht land the generated light whore dispersion of atoms and low chiged ions can compensite lage plasma dispersion a Regime IIA according othe presen invention. As discussed with rexpoct to FG. 4A, pase matching i achieved ay 8 isprsion balance etween atom and low-charged ions in & highly ionized medium 0091] FIG, 6B isa detailed schematic How digran illo tating the reduced phase velocity mismsteh where dispersion ‘of atoms and multiply charged ions can mitigate lmacr plasma dispersion in Regime IIB aeording to the present Invention. As dibcused with expect FIG. 4B, fll balance ‘eno! be achieve but te phase mismatch s minimized by ‘counterbulancing dispersion of stom and multply-125 ‘attosecond before compression. If the laser intensity in Rogime Ils increased fier, the eiep ean be decreased 10 ‘even smaller values, inversely proportionally to the lasee [0107] FIG. 14is plot of BG phase matching limits for prior art Regime IT (right-hand sie of figure) and efficient HIG upconversion photon energies in Regimes IIA and IIR ‘aeconling othe present invention (left-hand side of figure) FIG. 14 illustrates that using longer laser wavelength and Tightly ionized atoms, bright coherent soft and hard X-rays ‘can be generated (prior art, Regime Il). Acconling to the present invention (Regime IID, using shorter laser wave- Jengths and flly- or multiply-charged ions, brit soft and hard X-raysean be geneeated, While Regime ITA may extend the effcien upconversion mostly in the VUV-EUV region, Regime IIIB can extend the emission wel into the X-ray region, The two approaches in Regime Il and Regime IL are ‘complimentary t each other. The fist one generates prefer- ably coherent, supercontinuum, X-ray harmonics ideal for spectroscopic type of applications, while the second gener- ‘les preferably coherent ‘iy harmonics ideal for maging type of applications 10108] FIG. 184 is a plot showing example experimental ‘data demonstrating spectrally selected bright diserete har ‘monies in the X-ray region of the spectrum up to the water indow in Regime IIB according to the present invention (linear intensity scale. Experimentally observed UV-diven HHG extends up tothe water window at 280 eV, for laser intensities of 610! Wem’. FIG. ISA linear inteasity scale. [0109] FIG. 158 is plot showing example experimental ‘daa presenting brig dserete hamonie spanning the VUV- FUVX-ray spectral regions (log intensity seal). The plot show all the generated VUV-FUV-X-ray diserete narrons= band hamonics except for the 3” harmonic. Calculation show that the emission above 30 eV must originate Irom multiply charged ions (Ar*- Ar. [0110] FIG. 16isapiotshowing example experimental data demonstrating ultra-bright discrete harmonics in the EUV. spectral region in Regime IIIA aecording othe present inven: tion, FIG. 17 isa plot showing an example calculation ofthe 80 enhancement fora 0.4m diver compared to phise-mached emision fora 0.8 jn driver. Th total enhancement is de to an enbanced, favor able macroscopic pase matching, aswell 10 a favorable iroseopie yield (0114) FIGS. 194, B and C illsteate embodiments where Jsolte single harmonies of few hannonis are generated ‘sing a combination of low-pass filters and high-pass ites ‘This approach is attractive fom application point of since itmay redace the bani equrement or may con pletely eliminate the need for multilayer VUV-BUV:X-ray ‘rors that intoducesiiicant loss to select a single bare ‘monic. Using Teele driving pulse in principle ean also ‘esl in spect supercon comesponding (0 an so- fated VOY, BU or X-ray pulse [0115] FIG. 194 is plot showing example experimental data demonsrating beam profile and 2 bright nartow-band EUV harmon slated by tow-pas and high pas hi Hn fitters and by using a specifi laser intensity. FIG. 194 dem cnsirates a lated, single, 13am EUV Baroni (97 6) ‘ith nero newith of 7./4.~250 or >380 meV. The inst Shows the 13 am HHG beam, The adjacent harmon orders ‘wer filtered out using RheSieBe filters of solocted thick: [0116] FIG. 198 is a plot shossing example experimental ata demonstrating two Isolated, FUV harmonies around 13 ‘am with narrow linewidths. The adjacent harmonic orders ‘were filtered out using Rh+Be filters of selected thicknesses. [0117] FIG, 19C isa plot showing example experimental {data demonstratinga bright narrow-band VUV harmonie iso- Jated by low-pass and high pass thin fm fers and by using a specific laser intensity. The plot demonstrates isolated, Single, VUV huirmonies around 54 am (23 eV) with narow Tinewidth of ¥/A9.~300, The adjacent harmonic onders were ‘tered ou using an Sn iter of selected thicknessUS 2015/0063385 Al [0118] FIG. 20A is a plot showing an example of an ‘extended temporal window of elicient upconversion over 3 Jarge numberof driving laser cycles for Regime IT according to the present invention. [0119] FIG.208 (Prior Ar) plotshowing an example of f narrow temporal svidow of upconversion for prior art Regime 10120] Calculated ratio ofthe dynamic phase mismateh due ‘o plasma and tomisions for mult-6x10!? Wien. [0125] Using « 0.27 wm laser and very high laser intensity 26x10" Wen, bright emission fom mulkiply charged Ar fons ean extend up othe water window at >280 eV (Regime TIL), Note thatthe optimal pressure increases to above 400 ‘ore forthe highest X-ray harmonics. In comparison, using a OSym laserin Regime, the optimal pressure foranan-pase patched IHG from multiply charged Ar ions is 2 orders of ‘magnitude lower —-I-S tor Since the coherence length ia ‘Regime III nereases much slowly with burmonie order and the same photon energy corresponds to a loswer harmonic ‘order compared t Regime I, higher optimal pressures can be allowed. As mentioned show, a shorter coberence length ia ‘Reime I can lea ta bright HG emission also because of strong emission from a single atom, Furthermore, as highly charged states are generated during the laser pulse fora spe- cific temporal window the absorption of the medium related ‘o the fully ionized states can be reduce. ‘What is claimed is 1. The method of generating coherent emission within the \VUV, BU, and X-ray region oF the specteum comprising the steps of (@) providing a nonlinear medinm comprising a gas for high harmonic generation (HG) of laser light: (selecting the pressure ofthe nonlinear medium; (©) generating laser driving pulse having selected wave length within the VUV-UV-VIS region ofthe specteam anda selected peak intensity above 5x10!* Wem? and (@ focusing the driving pulse into the oalinear medium to ‘catine HIG upeonversion resulting in a generated pulse Wwithina selected range within he VUV, EUV, and X-ray region ofthe spectrin: ‘wherein the steps of selecting the medium pressure and ‘generating the driving pulse having the selected wave- Fength and the selected peak intensity effectively phase match the driving pulse and the generated pulse sufi ciently to result in @ coherent generated pulse wherein the coberence length is comparable to the absorption depthUS 2015/0063385 Al 2. The method of claim 1 wherein the selected wavelength and the slected peak intensity of the driving pulse result ia significant ionization ofthe nonlinear medium, ‘3. The method of claim 2 wherein the ionization of the nonlinear medium isa least about 10%, 4. The method of claim 3 wherein the nonlinear medium is fully ionized. 5. The method of claim 3 wherein the nonlinear medium is nutiply ionized (6, The method of claim § wherein the ionization of the nonlinear medium exceeds 300%. 7. The method of eluim 1 wherein the laser pulse has a ‘wavelength below 0.7 im, '8. The method of cluim 7 wherein the laser pulse has ‘wavelength of about 04 um, 9, The method of claim 7 wherein the laser pulse has 3 ‘wavelength of about 0.27 jm. 10, The method of claim 1 wherein the noolinear medium js multiply ionized and wherein the coherence length is at Teast about 1 yu TL, Themthod ofelaim 1 wherein the eoherence length is ‘atleast bout 0.5 em, 12, The method of claim 1 wherein the medium is one of the following: an atomic gas, a molecular gs, a mixture of mic gases, a mixture of molecular gases, a mixture of ‘atomic and molecular gases. 13. Themethod of claim 12 wherein the medium comprises ‘one of te flowing: He, Ne, Ar, Kr, Xe, Hz a 14, The method of claim I wherein the step of generating @ Jaserpulse generates pulse having aduration of between 600 attoseconds-1 picosecond and an energy of between 100 jd ‘and 1. 15. The method ofelaim 1 wherein the step of generating harmonic pulse penerates a pulse having a duration within the emtoscoond to zeptosecond range. Mar. 5, 2015 16, The method of elim 1 where the step of generating harmonics generates a comb of narrow-band hannonics 17. The method of claim 16 wherein the step of generating harmonics generates an isolted harmonic, 18, A method for global flix optimization of coherent harmonic emission at desired wavelength comprising the steps of () evaluating the total index of refraction of neutral and jonie species of # medium as e function of the wave= length of the diving laser and evaluating the index of refraction of the corresponding generated light; (b) evaluating the total index of refraction of neutral and onic species of a medium at a laser wavelength as 3 function of the time within the deving laser pulse (©) evaluating the (effective) HHG phase matching limits ‘as function of the laser wavelength; (@ determining the optimal laser parameters a a function ‘ofthe laser wavelength (©) evaluating the fax froma single emiterasa funetion of the driving laser parameters under (effective) phase matching conditions; (D evaluating the optimal density-length prodet as a fune- tion ofthe laser wavelength; (g) combining steps (a)() forthe purpose of ealewating ‘the macroscopic (effectively) phuse-matched coherent ‘emission asa function of the wavelength of the gener- ated Hight and the deving laser Tight and (finding the global maximum of the Mux at desired HG ‘wavelength forthe purpose af selecting optimal driving laser wavelength, optimal laser pulse parameters, opti= ‘ul spatial and temporal pulse shape, optimal nonlinear ‘medium and parameters ofthe nonfinear medi,