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Ultrafastlasersmode-lockedbynanotubesandgrapheneZ.
Sunn,T.
Hasan,A.
C.
FerrariDepartmentofEngineering,UniversityofCambridge,9JJThomsonAvenue,CambridgeCB30FA,UKarticleinfoArticlehistory:Received16January2012Accepted17January2012Availableonline25January2012abstractUltrafastlasersplayanincreasinglyimportantroleinmanyapplications.
Nanotubesandgraphenehaveemergedaspromisingnovelsaturableabsorbersforpassivemode-locking.
Here,wereviewrecentprogressontheexploitationofthesetwocarbonnanomaterialsinultrafastphotonics.
&2012ElsevierB.
V.
Allrightsreserved.
1.
IntroductionUltrafastlasersareusedinavarietyofapplications,rangingfromopticalcommunications[1]tomedicaldiagnostics[2]andindustrialmaterialsprocessing[3].
Developmentofnewgainmedia(e.
g.
Ti:sapphire[1–4]),andmode-lockingtechnologies(e.
g.
Kerr-lensmode-locking[1–4]andSemiconductorSaturableAbsorberMirrors(SESAMs)[4–6])havechangedtheoutlookofultrafastlasersoverthepasttwodecades.
Theseadvances,inparticulartherealizationofnewmode-lockingtechnologies,havepushedtheapplicationsofultrafastpulsestoarealmbroaderthaneverbefore.
Nevertheless,currentmode-lockingtechnolo-giesstillsufferfromdrawbacks,e.
g.
,Kerr-lensmode-lockedlasersusuallyrequireexternalperturbationsinordertostart[1,3,5]andareextremelysensitivetomisalignment[1,3].
SESAMsarecomplexquantumwelldevices,typicallyfabricatedbymolecularbeamepitaxyondistributedBraggreectors[4–8].
Post-growthprocessing[4–7](e.
g.
ionimplantation[4–7])isnormallyrequiredtoreducetheirresponsetime[4–7].
Theselimitat-ionsmotivateresearchonnewmaterials,noveldesignsandtechnologies.
Conventionallasers,includingion-dopedsolid-state,ber,semiconductor,liquidandgasbased,intrinsicallyhavealimitedwavelengthrangeofoperation[9],duetothelimitedtransitionsofthegainmedia[9].
Forexample,Ti:sappirelasersonlyworkbetween0.
65and1:1mm[9].
Nonlineareffects(e.
g.
opticalparametricgeneration[10,11]andRamanscattering[11,12])havebeenwidelyusedforlightamplication,inparticularforultrafastpulseamplication,duetobroad-bandgain,spectralrangeandgainbandwidththeyenable[11–13].
Forexample,Ramanampli-cation,wherebyasignalattheRamanStokes-shiftedwave-lengthexperiencesamplicationbystimulatedRamanscattering,isoftenemployedtoreachbeyondthespectrallimitsofrare-earthbers[9,14].
Ramanbasedamplicationcanpotentiallyallowbroadbandgainatanywavelengthacrossthetransparencywindowofsilica$3002300nm[9,14].
Withadvancesinhigh-powerber-laserpumptechnologyandincascadedRamanberlasers,highefcientpumpsystemsarenowavailableoverthisentireband,providingRamangaincoefcientsexceeding$70dB107[11].
Thesearchforalternativesaturableabsorber(SA)materials,essentialforpassivemode-locking[3–5,7],hasintensied,astraditionalSAs(e.
g.
organicdyes[15],colorlterglasses[16],ion-dopedcrystals[17])haveseverelimitationsintermsofstabilityandperformance(e.
g.
slowresponsetime[5],narrowoperationwavelength[7,18],expensivefabricationandintegra-tionmethods[5],lowdamagethreshold[5]).
Singlewallcarbonnanotubes(SWNTs)haveemergedasnewSAmaterialwithsuperiorperformance,suchassub-picosecondrecoverytime[18–25],mechanical[18,26]andenvironmentalrobustness[27,28].
SWNTmode-lockedultrafastlasershavebeendemon-stratedforvariousapplications(e.
g.
industrialmeasurements[29],materialprocessing[28],opticalsampling[30],data-patternrecovery[30],opticalfrequencymetrology[31,32],andopticalcoherencetomography[33]).
GraphenehasalsocometotheforeasanewSAwithultrafastrecoverytime[34–39]andultra-broadbandoperation(Fig.
1(a,b))[18,38–41].
2.
SWNTmode-lockedlasersSWNTbasedSAs(SWNT-SAs)havebeensuccessfullyimplemen-tedinavarietyoflaser:solid-state[42–48],ber[18,27,28,49–72],semiconductor[73]andwaveguide[74,75].
VariousstrategieshavebeenimplementedtofabricateSWNT-SAs,Table1.
Theseincludespraycoating[49,50,73,76–82],directgrowth/transfer[57,59,83–86],opticallydrivendeposition[27,28,51–53,61,62,68–70,74,87–90],polymercomposite(Fig.
1(a))[27,28,51–53,61,62,68–70,74,87–90],polymerber[91].
ContentslistsavailableatSciVerseScienceDirectjournalhomepage:www.
elsevier.
com/locate/physePhysicaE1386-9477/$-seefrontmatter&2012ElsevierB.
V.
Allrightsreserved.
doi:10.
1016/j.
physe.
2012.
01.
012nCorrespondingauthor.
E-mailaddress:zs244@cam.
ac.
uk(Z.
Sun).
PhysicaE44(2012)1082–1091DifferentapproacheshavebeenusedtointegrateSWNT-SAsinlasers,suchasfree-spacecoupling(Fig.
2(a))[49,50],depositiononberends[55,161]andinsidebers[67,92]aswellaseveanescenteldinteraction[56,66,81,84,93],Thusfar,themostpopularwaytointegrateSWNT-SAsintoberlasersistosandwichaSWNTpolymercompositebetweentwobercon-nectors(Fig.
2(b))[18,27,28,51–53,61,62,68–70,74,87–90],sincethisofferseaseofintegrationintovariouslightwavesystems[18,27,28,51–53,61,62,68–70,74,87–90].
Alargerangeofhostpolymers,e.
g.
polycarbonate(PC)[51,64,75,94,95],polyvinylalcohol(PVA)(Fig.
1(a))[27,28,52,53,61,62,68–70,74,87–90,96–98],Carboxymethylcellulose(CMC)[47,42,43,71,99–104],Polyimide(PI)[42,63,105,106],Polydimethylsiloxane(PDMS)[65,66,107–109],Polymethylmethacrylate(PMMA)[44–46,48,60,92,110–112]andpoly(3-hexylthiophene)(P3HT)[113–115],havebeenused.
SWNTsutilizedinSAshavebeenpreparedusingavarietyofgrowthtechniques,e.
g.
laserablation(LA)[27,28,42,49–51,61–64,68–70,74,75,90,94,96–98,102,105],arcdischarge(AD)[44,45,71,103,104,110,116,117]andvariousche-micalvapordeposition(CVD)methods[118,119](suchasCobalt–Molybdenumcatalyst(CoMoCAT)[42,52,53,87–89,115],HighPressureCarbonMonoxide(HiPCO)[43,46–48,55,60,65–67,76–78,81,86,92,95,99–101,107,108,111–114,120–125]andalco-holcatalyticchemical–vapordeposition(ACCVD)[59,83–85]),allow-ingtheselectionofdifferentdiametersanddiameterdistributions.
Sincetherstdemonstrationin2003[49],theperformanceofultrafastlasersmode-lockedbySWNTshassteadilyimproved.
Table1summarizesrepresentativeoutputperformances.
Forexample,theaverageoutputpowerhasincreasedfromfewhundredmw(e.
g.
$260mw[50])tofewWatts[28,108,126],withpeakpowersreachingafewhundredkW(e.
g.
200kWinRef.
[120]).
Alargerangeofoutputparameters,suchaswavelength,pulseduration,andrepetitionratehavebeenachieved.
Thusfar,thedemonstratedwavelengthsrangefrom0.
78[47,127]to2mm[57,71,110,128].
Theoutputpulsedurationsrangefromafewns[52,53]tosub-20fs[107].
TherepetitionratespansfromfewtenskHz[52,53,129]toafewtensGHz[73,130].
Wavelength-tunablelasersbasedonSWNTshavealsobeenreported[47,51,63,98,128,131–134].
2.
1.
SWNTmode-lockedsolid-statelasersSolid-statelasers,mainlyusingdopedglass[3,10]orcrystal-linehostmaterials[3,10]asgainmedia,arethemostcommonlyusedinvariousapplications(e.
g.
industry,researchandmilitary[3,10,11]).
Theytypicallyconsistofafree-spacecavity,formedbymirrorsandasolid-stategainmedium[178].
Avarietyofsolid-stategainmediahavebeencoupledwithSWNT-SAstomode-locksolid-statelasers.
TheseincludeNd:glass[42,43,152,157],Nd:GdVO4[99,135,171],Nd:YVO4[117,126,137,155,172],Nd:YAG[100,101,158],Nd:YLF[170],Nd:LuYVO4[136],Er:glass[42,82,122],Yb:Sc2SiO5[173],Yb:KLu(WO4)2[44,45],Yb:KYW[46],Yb:LuYSiO5[174,175],Yb:LuScO3[179],Cr:YAG[46,133],Cr:LiSAF[134],Cr:forsterite[46,48]andTm:KLu(WO4)2[110].
Inparticular,SWNT-SAshaverecentlybeenreportedtomode-locksolid-stateTi:sapphirelasers[47,127].
Thisisanimportantstep,sinceKerr-lensmode-lockedTi:sapphirelasersdominatethesub-200fsmarket.
However,Kerr-lensmode-lockingisnotself-starting[1,11]andusuallyrequirescriticalcavityalignment[1,3–5].
TheoutputspectraofSWNTmode-lockedsolid-statelasershavethusfarcovered0.
8[47,127,134],1[42–46,179,175],1.
2[46,48],1.
3[99–101,155],1.
5[42,46,82,122,133]and2mm[110].
SWNTsarenormallycoatedonhighreectivitymirrors[42,44,46,82,134],andthenemployedascavitymirror.
Hightransmittancesubstrates(e.
g.
purequartz[45,100])coatedwithSWNTs(Fig.
2(a))havealsobeenused[45,100,133,126].
Theshortestpulsedurationthusfarachievedis$60fs[42,127].
High-powerupto3.
6Wwasreportedat1:06mm[126,135].
Comparedtoberlasers,optimizationoftheSAnon-saturablelossesiscrucialtomode-locksolid-statelasers[3,46],sincetheirgainislower,mainlyduetothelimitedgainmediumlength(severalmm)[3,10].
Forwide-bandoperation,SWNTscoveringavarietyofdiametersneedbecombinedtoformtheSAdevice.
Thesetubes,however,tendtobundleandcurl[18,46],thuscontributingtohighnon-saturablelosses[18].
Recently,asingleSWNT-SAwasusedtomode-locksolid-statelasersat1,1.
2and1:5mm[46],showingthatnon-saturablelossesmaybedecreasedbyoptimizingtheSWNT-SAfabrication.
2.
2.
SWNTmode-lockedberlasersFiberlasersareattractivealternativestobulksolidstatelasersduetotheirefcientheatdissipation[3,13]andalignment-freeformat[3],thelatterbeingakeyadvantageforend-users.
Furthermore,theirtypicalgaincanreachseveraltensdB[11],afewordersofmagnitudehigherthansolidstatelasers[10,11].
Thus,theydonotneedparticularoptimizationofnon-saturablelossesfortheiroperation,asthelosscanbecompensatedbythelargegain.
Indeed,therehasbeenafargreaterresearcheffortonexploitingSWNT-SAsinberlasers,asevidentfromTable1,withasteadyimprovementinperformance.
Atypicalmode-lockedberlasersetupisshowninFig.
2(c).
Thisunidirectionalringcavitydesignallowseasyself-startingduetodecreasedspuriousreections[180].
Themaximumreportedaverageoutputpoweris$250mW[84],with6.
5nJoutputpulseenergyat$1:5mm[84].
InRef.
[84]SWNTsweretransferredonaD-shapedbertoenableevanescenteldinteraction,atechniquealsoreportedinRefs.
[56,66,81,93].
Normal-dispersionberlasers[28,52,53,88,145,112]havealsobeendemonstrated,Fig.
1.
(a)AbsorptionofSWNTandgraphenepolymercompositeSA.
Inset:micrographofagraphenepolymercomposite.
(b)TypicalGSAtransmittanceasafunctionofinputpoweratdifferentwavelengths,adaptedfromRef.
[38].
Z.
Sunetal.
/PhysicaE44(2012)1082–10911083Table1PulsedlasersexploitingSWNT-SAs.
l:wavelength;t:pulsewidth;f:repetitionrate;P:averageoutputpower.
SAsSWNTtypesLasertypesLaserparametersl(nm)tf(MHz)P(mW)PolymercompositesPCLA[51,64,75],HiPCO[95]EDFL[51,64,95],waveguidelaser[75]1518–1558tunable[51],1560[64,75,95]115fs[95],2.
4ps[51]15[51],39[95]0.
36[51],3.
4[95]PVACoMoCAT[52,53,87,88],LA[27,28,61,62,68–70,74,90,96–98],AD[135,136],HiPCO[125]Nd:YVO4[137],Nd:GdVO4[135],Nd:LuYVO4[136],YDFL[52,53,87,138],BDFL[88],EDFL[27,28,61,62,68–70,90,96–98,125,139–142],Waveguidelaser[74]1058–1060[52,53,138],1530–1563tunable[98],1532–1563[27,28,61,62,68,69,74,90,96,97,125,139,140,142],1601[70]113fs[69],20ps–2nsselective[52,53,87]0.
177–21selective[52,53,87],328[141]0.
1[74,90],3.
6W[135]CMCCoMoCAT[42],HiPCO[43,47,99–101,143,144],LA[102],AD[71,103,104,145,146]Ti:sapphire[47,143],Nd:glass[42,43],Nd:GdVO4[99],Nd:YAG[100,101],YDFL[144–146],EDFL[102–104,144,146–149],TDFL[71]780–820tunable[47,143],1000–1068[42,43,144–146],1320–1340[99–101],1550–1565[102,104,144,146–149],1930[71]177fs[104],1.
15ns[145]37[71],110[47]3.
4[71],450[47]PILA[42,63,105,106,150],HiPCO[65]Er:glass[42],EDFL[63,105,106,118,119,150]1532–1562tunable[63],1532and1557Switchable,1545–1570[42,105,106,119,150]68fs[42],6.
2ps[150]0.
13[150],85[42]0.
4[150],114[106]PDMSHiPCO[32,66,107–109,128,151]EDFL[32,66,93,107–109,151],YDFL[56],TDFL[72,128]1035[56],1530–1565[66,93,107,108,151],1885[72],1866–1916tunable[128],1000–1750[107,108]14fs[107],1.
5ps[56]13.
3[66],4GHz[109]1[93],11.
5[108]PMMAAD[44,45,110,152],HiPCO[46,48,60,92,111,112,127,134,153–155]EDFL[60,91,92,111,112,154],Yb:KLuW[44,45],Yb:KYW[46,131],Nd:BaYF[156],Nd:Glass[152,157],Nd:YVO4[155],Cr:forsterite[48,46,153],Cr:LiSAF[134],Ti:sappire[127],Cr:YAG[46,133],Tm:KLuW[110]780–825tunable[127],868–882tunable[134],1035–1045tunable[131],1061–1075tunable[157],1048–1080[44,131,152,156],1240–1250[48,153],1342[155],1435–1505[133],1560–1567[60,91,92,111,112,154],1944[110]62fs[127],9.
7ps[110]5.
3[111],1.
69GHz[112]50mw[60],800[155]P3HTHiPCO[113,114]CoMoCAT[115]EDFL[113,114],YDFL[115]1070[115],1560[113,114]113fs[114]51[113]5[114]PFO//Nd:YAG[158]1064[158]8.
3ps[158]90[158]275[158]PSHiPCO[60]EDFA[60]1560[60]171fs[60]7.
63[60]0.
050[60]SU8HiPCO[159]EDFA[159]1571[159]871fs[159]21.
27[159]1[159]Grown/deposited/transferredSWNTsOpticallydrivendepositionHiPCO[55,120,121,160],CoMoCaT[55]YDFL[55],EDFL[55,120,121,160–163]1070[55],1532–1567[55,120,121,160–162]124fs[163],1.
14ps[121]5.
2[160]0.
1[55],1.
5W[120]Spray-coatingHiPCO[76–78,81,130],LA[49,50]PDFL[76],TDFL[80],EDFL[30,49,50,77,78,80,81,132,164],EYDFL[79,130],Er:Yb:glass[82],Semiconductorlaser[73]1294[76],1506[80],1550–1571[30,49,50,73,77–82,130],1605[80]190fs[164],14ps[73]3.
18[76],19.
4GHz[130]16mw[73],63[82]Grown/transferredACCVD[59,83–85],HiPCO[57,86,165–168]YDFL[57],EDFL[31,57,59,83–86,165–168],TDFL[57,167]1050[57],1550–1565[31,57,59,83–86,165,167,168],1990[57,167]30fs[31],1.
14ps[85]6.
62[85],50[59]22mw[85],250[84]Drop-castingAD[117,126,169–171],CVD[172–174]Nd:YLF[170],Nd:YVO4[117,126,172],Nd:GdVO4[171],Yb:SSO[173],Yb:LuYSiO5[174,175]1045/1059[174],1047–1064[126,169–171,173,175]1.
1ps[169],15ps[173]79.
7[117]280[170],3.
6W[126]Sol–gelglass//EDFL[176,177]1559–1563[176,177]0.
57ps[177],2.
3ps[176]2.
96[176]2[177]SolutionCellHiPCO[122,123]Er:glass[122],F2:LiF[123]1150[123],1540[122]o1ns[122]////Micro-channelHiPCO[67,124]EDFL[67,124]1566[67]0.
9ps[124],2.
3ps[67]2.
56[67],5.
26[124]15[124],22.
4[67]Z.
Sunetal.
/PhysicaE44(2012)1082–10911084with155mWaverageoutputpowerand3nJpulseenergyat$1:03mm[56].
Ref.
[102]reported63nJpulsegeneration,thehighesttodatefromaSWNT-SAenabledultrafastlaser.
Ref.
[181]theoreticallypredictedthatSWNTmode-lockedberlasercouldachieveupto330nJ.
TheshortestpulseachievedthusfarfromSWNT-SAmode-lockedberlasersis$84fs[182],byusingastretched-pulsedesign[69],i.
e.
alternatingnormalandanomalousdispersion,toobtainperiodicstretchingandcompressionoftheintracavitypulsesintheresonator[69,183].
Thus,theaveragepulsewidthinonecavityroundtripcanincreasebyanorderofmagnitudecomparedtothetypicalsolitiondesign[69,183],andultrafast(e.
g.
77fsfromanonlinearpolarizationevolution(NPE)mode-lockedErbium(Er)dopedberlaser(EDFL)[183])pulsesareachievableduetothereducednonlineareffects[69,183].
Atypicalautocorrelationtraceofastretched-pulseberlaserisshowninFig.
3(a).
Selectablepulseduration,from20psto2ns,wasalsodemonstratedbychangingcavitylength(showninFig.
3(b))[52,53].
Ashortcavitydesign[79,130]andharmonicmode-locking(wheremultiplepulsescirculateinthelaserresonatoratanintegermultipleofthefundamentalfrequency[11])canallowhighrepetitionrate.
Ref.
[130]reportedSWNTmode-lockedpulsesupto$20GHz,usingacavityformedbya$5mmbersandwichedbetweentwomirrors.
Severalgainbreshavebeenusedtodate,includingYtterbium(Yb)doped(YDFL)[52–57,146],EDFL[27,28,54,55,57,59,61,62,64,67–69,109,112,125,146,184],ErandYbco-doped(EYDFL)[54,130],Bismuth(Bi)doped(BDFL)[88,89],Praseodymium(Pr)doped(PDFL)[76]andThulium(Th)doped(TDFL)[57,71,72].
Amongstthem,EDFLsarethemostpopular,sincetheyalloweasyexcitationofsolitonpulsesinsinglemodebers[3],andallnecessarycomponentsareeconomicallyavailablefromtheber-telecommarket[3].
Theachievedwavelengthrangecovers1[52–57],1.
1[88,89],1.
3[76],1.
5[27,28,49,50,57–69],1.
6[70],and2mm[57,71,72].
Ref.
[51]rstdemonstratedwavelength-tunabledevices.
Later,byusingasingleSWNT-SAdevice,Ref.
[57]achievedmode-lockingat1,1.
5and2mm,inYDFL,EDFLandTDFL,respectively.
Wide-bandoperationrequiresthecombina-tionofSWNTswithdifferentdiameters[18,51,57].
Ref.
[146]demonstratedthesynchronizationoftwoall-bermode-lockedlasers,operatingat$1and1:54mm,coupledthroughasharedSWNT-SA.
Refs.
[185–188]reportedRamanberlasersmode-lockedbynanotubesat1.
1[187,188]and1:6mm[185,186],whenpumpedat1and1:5mm,respectively.
PulsesfromSWNTmode-lockedberlasershavealsobeenusedforfurtherinvestigations,e.
g.
nonlinearcompression[65],amplication[28,31,32,108,120]andsuper-continuumgenera-tion[31,107,108,130,189].
Anoutputaveragepowerofupto1.
6WhasbeenachievedbyusingdirectamplicationofaSWNTenabledchirp-pulseoscillator[28],withthepotentialforfurtherscalingofoutputpower/pulseenergy[28].
11.
5Wpulseswerereportedwiththreecascadedampliers[108].
Afterthegratingcompressor,135fspulsesweregeneratedwith5.
7Woutputpowerand160nJpulseenergyinRef.
[108].
Notethatintheseamplicationexperiments[28,108],theoutputpowerisjustlimitedbythepumppower,i.
e.
evenhigherpowercouldbepossiblebyincreasingthepumppower.
Ref.
[31]seededtheoutputpulsesfromaSWNTmode-lockedoscillatorintoanFig.
2.
(a)Graphenepolymercompositecoatedonaquartzsubstrate.
Itstransparencytolight(indicativeoflowloss)makesthissuitableforintegrationinsolid-stateandwaveguidelasers(b)Integrationofagraphenesaturableabsorberpolymer-compositelmbetweentwoberconnectorsforberlasers.
Notethattheseintegrationmethods(asshownin(a)and(b))alsoapplytoSWNT-SAintegration.
(c)Typicalpassivelymode-lockedberlasersetup.
WDM:wavelengthdivisionmultiplexer;ISO:isolator.
Fig.
3.
(a)AutocorrelationtraceofoutputpulseswithGaussiant.
(b)Outputpulsedurationasafunctionofcavitylength,adaptedfromRef.
[52].
(c)Tunablemode-lockedberlaserspectra,adaptedfromRef.
[40].
Z.
Sunetal.
/PhysicaE44(2012)1082–10911085amplier,followedbyahighlynonlinearber,tobuildaberlaserbasedfrequencycomb(i.
e.
alightsourcewithopticalspectrumconsistingofequidistantlines[11]).
Supercontinuumgeneration(anonlinearprocesstostronglybroadenthespectrumoflight[11])hasbeendemonstratedwith30-fsoutputpulses[31].
Usingsupercontinuumgeneration,Ref.
[107]reported14fspulsesbyseedingaSWNTmode-lockedberlaserintoanon-linearber,withoutputspectrumcoveringfrom1to1:75mm.
2.
3.
SWNTmode-lockedsemiconductorlaserSemiconductorlasersusuallyexploitdirectbandgapsemiconduc-torsasgainmedium[11].
Sincesuchlaserscanbeelectricallypumped[11],theyhavebeenwidelyemployedinarangeofcommondevices,fromhomeentertainment[190](e.
g.
CD/DVDplayers)totelecommunications[11].
Furthermore,semiconductorlasersareattractivealsobecauseoftheirinherentsimplicityandcompactness[11].
Theoutputpulserepetitionrate(frep)islinkedtothecavitylength(L)byfrepc=2nL,wherecisthespeedoflight,andnistherefractiveindexofthecavitymaterial[1].
Therefore,mode-lockedsemiconductorlaserstypicallyofferhigh4GHzrepetitionrateduetotheirrelativelyshort($afewmm)cavitylength.
Consequently,mode-lockedsemiconductorlasersareparticularlysuitableforhigh-speedopticalcommunications[1].
Ref.
[73]rstdemonstratedaSWNT-SAmode-lockedsemiconductorlaserwithrepetitionrateupto17.
2GHz,usingasemiconductoropticalampliertoprovidegainat$1:5mm.
Thefullwidthathalfmaximum(FWHM)ofthepulseswas0.
73nmat$1570nm,withaduration$14ps[73].
2.
4.
SWNTmode-lockedwaveguidelasersSolid-statewaveguidelasersarebuiltonplanarorchannelwaveguidesinpolymer,glassorcrystallinesubstrates[11].
Passivemode-lockingofwaveguidelasersisalsoinherentlysimpleandcompact.
Comparedtotraditionalsemiconductorlasers(havinganupper-statelifetimeintheorderofns[190]),solid-statewaveguidelasersaremoresuitableforhigh-energypulsegeneration,becausethegainmaterialstypicallyhavelongerupper-statelifetime($ms)[11].
Therefore,moreenergycanbestoredinsidethegainmaterialforhigh-energypulsegeneration[10,11].
Avarietyofdevices,suchaswaveguides[191],couplers[192],gratings[193],opticalampliers[194]andoscillators[194]havebeenfabricatedbyultrafastinscriptionintransparentsubstrates,atechniquenotneedinganyphotolithographicpro-cess,andallowingthree-dimensionaldevicefabrication[194].
Ref.
[74]rstdemonstratedmode-lockingwithaSWNT-SAinanactivewaveguidelaserfabricatedbyultrafastlaserinscription.
AnErandYbco-dopedphosphateglasswaveguidewasused,providingnetgainoverthewholetelecomCBandand7.
3dB$5:4peakgainat1535nm[74].
Thelasergenerated1.
76pstransform-limitedpulses[74].
Recently,bismuthateglasseshavebeenemployedaswave-guidegainmedia,astheycanbedopedwithsufcientconcen-trationsofEr-ionsforhighgain.
Ref.
[195]reportedthatabismuthatewaveguideampliercanexhibitapeaknetgain$16dB$40at1533nmandawideandatgainspectrum[195],favorableforultrafastpulsegeneration[11].
Ref.
[75]achieved320fspulsesinanEr-dopedbismuthateglasswave-guidelasermode-lockedbyaSWNT-SA,withanoutputspectralwidth$8:9nmat1:55mm[75].
3.
Graphenemode-lockedlasersGrapheneisatthecenterofanevergrowingresearcheffortduetoitsuniqueelectronicproperties[230–236].
Near-ballistictransportatroomtemperature[231,237]andhighmobility[234–238]makeitapotentialmaterialfornanoelectronics[238–241],especiallyforhighfrequencyapplications[238–241].
Furthermore,itsopticalpropertiesareidealfortransparentconductinglms[39,242,243]andelectrodes[39,244],photode-tectors[39,245,246]andopticalmodulators[39,247,248].
Theultrafastnonlinearpropertiesofgraphenehavebeeninten-sivelyinvestigated[34–37].
Tworelaxationtimescalesaretypicallyobserved.
Afasteroneo100fs,usuallyassociatedwithcarrier–carrierintra-bandcollisionsandphononemission[34,36,37],andaslowerone$ps,correspondingtoelectroninter-bandrelaxationandcoolingofhotphonons[34–37,39,249].
GrapheneisthusanultrafastSAmaterial[18,38,39].
Ref.
[18]rstreportedaGSAmode-lockedlaser.
Subsequently,avarietyoflasersmode-lockedbygrapheneweredemonstrated[38–41,200,201,203–205,207,208,214,216,226],asshowninTable2.
Graphenehasbeensourcedinvariousways,suchasliquidphaseexfoliation[18,38,40,199],CVD[200,201,203–205],carbonsegregation[218],grapheneoxide,GO,[39,208,221]),reducedGO[214,216]andmicro-mechanicalcleavage[39,209–211].
AsshowninTable2,severalapproaches(e.
g.
sandwiching[18,38],free-spacecoupling[216,227],placementinsidePhotonicCrystalFibers(PCFs)[215],evanescenteldinteraction[214])havebeenusedtointegrateGSAsintocavities,mostlyfollowingpreviousapproachesusedforSWNT-SAs.
SandwichingaGSAbetweentwoberconnectors(Fig.
2(b))isthusfarthemostcommonapproachforGSAintegration[18,38,40,41,200,201,203–205,207,208,210].
ComparedtotraditionalSAs(e.
g.
SESAMs)andSWNT-SAs,themajoradvantageofusinggrapheneistheintrinsicwide-bandoperation.
Thusfar,GSAshavebeenusedtoproducepulsesat1[216],1.
25[226],1.
5[18,38–41,199–201,203–205,207,208,210,214],and2mm[225,250].
SimilartoSWNT-SAs,GSAshavebeenmostlycombinedwithEDFLs[18,38,40,41,199–201,203–205,207,208,210,214],notbecauseGSAshaveanypreferenceforaparticularwavelength,butbecauseEDFLscaneasilyproducesolitonpulsesinsinglemodebers[3],andallnecessarycomponentsareeconomic-allyavailablefromtheopticaltelecommarket[3].
Ref.
[40]reportedGSAmode-lockedberlaserstunableinthe1525–1559nmrange(Fig.
3(c)),onlylimitedbythelterusedinthecavity[39,40].
Ref.
[205]reported$240fstunablepulsegenerationusingberlasersunderdifferentoperationregimes(e.
g.
fromall-anomaloustoall-normaldispersion).
Stretched-pulsedesignwasemployed,generatingsub-200fspulses[196].
Ref.
[251]reported163nJpulsegenera-tion.
Refs.
[216,221,220,224–227]alsoreportedpulsesusingsolid-statelasersmode-lockedbyGSAs.
94-fstunable$1:221:27mmpulseshavebeenachievedwithaGSAmode-lockedsolid-stateCr:forsteritelaser[226].
High-power$1WpulseshavebeendemonstratedwithaGSAmode-lockedNd:YVO4solid-statelaser[220,221].
4.
OutlookCurrently,solid-stateandberlasersarethemostcommonforhighoutputpower/pulseenergyapplications[1,3].
Amongstvarioussolid-statelasercongurations,athin-diskdesigncansignicantlyreducethermaleffectsandnonlinearities[252],enablinghighaveragepowerandenergypulses[252,253].
SWNT-SAsandGSAscouldbeusedinthin-diskdesignsforthispurpose.
Themainchallengeistherelativelylargenon-saturablelossoftheseSAs,whichcanbeaddressedbyfurtherdeviceoptimization(e.
g.
enrichmentinsemiconductingnanotubes[18]).
Theoutputpeakpowerofberlasersisrestrainedbyenhancednonlineareffects[1,3,254].
Recently,large-mode-areaberbasedultrafastlasersworkinginadissipativesolitonregimehavebeendemonstratedforhighaveragepowerpulses[255,256],Z.
Sunetal.
/PhysicaE44(2012)1082–10911086Table2PulsedlasersusingGSAs.
LPE:liquidphaseexfoliation;GO:grapheneoxide;FG:functionalizedgraphene.
CS:carbonsegregation.
MMC:micro-mechanicalcleavage.
RGO:reducedGO.
LasertypeCouplingmeansFabricationmethodLaserparametersRef.
l(nm)tf(MHz)P(mw)EDFLSandwichingLPE1557800fs////[18]1559464fs19.
9//[38]1525–1559tunable1ps81[40]1560174fs27.
41.
2[196]1562630fs19.
9//[41]1522–1555tunable2ms0.
036–0.
13.
4[197]1519–1569tunable4:6ms0.
008–0.
0292.
4[198]1532850fs5.
27//[160]1565190fs42.
80.
4[199]CVD1565756fs1.
792[200]1576415fs6.
8450[201]15611.
23ps33[202]15942.
1,71ps////[203]1570–1600tunable40–140ps1.
5//[204]1570–1600tunable240–655fs,70–150ps////[205]1538206ns0.
031–0.
2367.
8[206]FG1559743fs////[39]1590700fs6.
9550[207]1570–1600tunable1.
08ps6.
95//[208]MMC//3.
2ps10.
93[209]15660.
88ps6.
22//[210]1561480fs7//[211]RGO1566.
1/1566.
33:718ms0.
003–0.
0651.
1[212]1572.
6//91.
5//[213]Evanescenteld15611.
3ps6.
9915.
5[214]PCFFG15614.
85ns7.
684.
3[215]Nd:YAGFree-spaceRGO10644ps88100[216]RGO1064260ns0.
1671389[217]CS1064161–400ns0.
3–0.
66105[218]Nd:LuVO4106456–131ns0.
89474[219]Nd:YVO4GO1063//751000[220]////881200[221]Nd:GdVO41064105–1435ns0.
3–0.
72300[222]106516ps43360[223]Yb:KGW1031428fs86504[224]Tm:YAlO32023$10ps71.
8268[225]Cr:forsteriteCVD1222–1227tunable94fs74.
6230[226]Er:Yb:glass1552260fs884.
5[227]YDFLSandwiching1069580ps0.
90.
37[228]LPE106470–250ns0.
14–0.
25712[229]Z.
Sunetal.
/PhysicaE44(2012)1082–10911087reachingMWpeakpowers[257].
Inprinciple,large-mode-areaberlasersmode-lockedwithSWNTsandgraphenemaydeliverbetterperformances(e.
g.
highaveragepower,highpeakpower,systemsimplicity).
Forexample,coatingSWNT-SAsandGSAsonthebersurfacestoenableevanescent-waveinteraction[56,84]orinsidethebers[67](e.
g.
holesofPCFs[92,215])canpreservethealignment-freewaveguideformatofsuchberlasers,byremovingthefree-spacecomponents,whicharenecessaryfortraditionalSA(e.
g.
SESAMs[257])coupling.
Theseintegrationstrategiescanbeappliedtovariouslaserdesigns,suchaswaveguide(e.
g.
laserinscribed[194]orpolymer[258])andsemiconductor(e.
g.
verticalexternalcavitysurface-emittingsemiconductorlasers[259]andopticallypumpedsemiconductordisklasers[260])forhighpower/energypulsegeneration.
ThistechnologycanalsoenablecompactlaserswithrepetitionratesuptohundredsofGHz[29,130].
Anotheroptiontoincreaserepetitionrateisviaharmonicmode-locking[1].
Thecombinationofwide-bandgainmaterials(forexampleTi:sapphire)andSWNT/grapheneSAscouldproducenovelbroad-bandtunableultrafastsources.
NotethatGSAscanintrinsicallyoperateat''full''bandwidth[18,38,39],whiletheoutputwave-lengthortuningspectralrangeofatraditionallaserwillbeultimatelyconstrainedbythegainmedium.
Nonlineareffects(e.
g.
opticalparametricgeneration[261,262]andRamanscatter-ing[9,14])canbeusedtobroadenthespectralrange.
Theycanprovidebroadbandgain,potentiallycoveringfromultraviolet[263]toterahertz[264].
TherecentdemonstrationofbroadbandRamangain[185–188]andbroadbandSWNT-SAs/GSAsshowsthepossibilityofgettingbroaderoutputspectrathaneverbefore.
ExternalamplicationofSWNTandgraphenemode-lockedlasers[28,31,108,120]orcoherentcombinationofvariouslasers[265–267]couldboostoutputpowerandenergy.
Nonlinearfrequencyconver-sion(e.
g.
harmonicfrequencygeneration[1,268–271],parametricoscillation[261,272,273]andamplication[1,262],four-wavemixing[11],supercontinuumgeneration[31,107,108,263,189,130])isalsoanusefulwaytoexpandthewavelengthaccessibilityaftertheoscillator.
External-cavitypulsecompression(e.
g.
nonlinearcompression[11,31,65,107,108])couldbeusedtogenerateshorterpulsedowntoafewopticalcycles(e.
g.
4.
3-fs[274]).
AcknowledgmentsWethankF.
Hennrich,F.
Wang,D.
Popa,F.
Torrisi,W.
B.
Cho,A.
Rozhin,V.
Scardaci,F.
Bonaccorso,Z.
Jiang,R.
Going,I.
H.
White,S.
J.
Beecher,R.
R.
Thomson,A.
K.
Kar,E.
J.
R.
KelleherandJ.
R.
Taylorforusefuldiscussions.
WeacknowledgefundingfromtheERCgrantsNANOPOTS,EUgrantsRODINandGENIUS,EPSRCgrantsEP/GO30480/1andEP/G042357/1,King'scollegeCambridge,theRoyalAcademyofEngineering,aRoyalSocietyWolfsonResearchMeritAward,andtheCambridgeNokiaResearchCentre.
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