Supplement of Exploring femtosecond laser ablation in single-particle aerosol mass spectrometry

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1 Supplement of Atmos. Mes. Teh.,, 35 30, 08 Author(s) 08. This work is istriute uner the Cretive Commons Attriution.0 Liense. Supplement of Exploring femtoseon lser ltion in singleprtile erosol mss spetrometry Rmkrishn Rmisetty et l. Corresponene to: Clui Mohr The opyright of iniviul prts of the supplement might iffer from the CC BY.0 Liense.

2 The supplementry informtion ontins informtion out lsermtter intertion t ifferent time sles, the numer of mss spetr mesure in eh experiment with ifferent lsers for ifferent prtile types, the soures of the ifferent prtiles types, the lultion of the lser em imeters n power ensities, n the supporting informtion for fslser spetrl seletion n reprouiility. 5 Time sles of lightmtter intertion 5 0 The lser ltion n ioniztion mehnism epens on the pulse urtion of the lser. Figure S (tken from Hm et. l. (0) () n Royon et l. (0) ()) shows the ltion mehnism for ifferent pulse urtions n time sles. Nnoseon lser ltion: The trget mteril surfe sors the energy n hets up, then therml vporiztion n ltion tkes ple. In ultrshort lser pulse ltion mutliphoton ioniztion, oulom explosion, therml vpouriztion n then plsm formtion tke ple. At ultrshort femtoseon lser intertion, two ifferent ltion regimes re oserve: ) non therml Coulom explosion upon multiphoton surfe ioniztion is the ominnt proess, yieling eletrons n fst ions. ) At higher lser intensities, ltion exhiits signs of hypertherml emission (phse explosion) s result of rpi hot eletron thermliztion. The fslser ltion mkes more tomi ions thn the nnoseon lser ltion ue to rpi energy trnsfer, ut lso mkes more ion lusters euse of the explosion proesess. Hene, fslser ltion genertes lrger ion lusters thn nslser ltion (Bulgkov et l., 00; Hrill et l., 0; Kto et l., 007; Royon et l., 0). These proesess re expline n oerserve well for fixe trgetlser intertions, however, they re rrely stuie for irorne prtiles (Murphy n Thomson, 995; Zwowiz et l., 05; Zhou et l., 007). Nevertheless, the physil mehnisms of the prtilelser intertions my e omprle espeilly for lrger erosol prtiles. 5

proesses hppening uring n fter the lser pulse is pplie.

3 30 Figure S : (Top) Approximte time sles of nnoseon n femtoseon energy sorption n lser ltion long with vrious proesses hppening uring n fter the lser pulse is pplie. (Bottom) Timesle of the physil phenomen involve in lightmtter intertion.

4 Tle S : Numer of prtiles mesure with nslaaptof with ifferent pulse energies t fous positions F n F. Typilly more thn 80 % of the spetr out of these re usle (nonempty spetr). Prtile types Dimeter ( p) nm Numer of spetr otine for three ifferent lser energies 0.8 mj mj 8 mj 35 t F t F t F t F t F t F PSL PSL PSL Sili NCl NH NO AuAg AuSiO AuPAH Tle S : Numer of prtiles mesure with fslaaptof with ifferent pulse energies t fous positions F n F. Typilly, more thn 0 % to 0 % of the spetr out of these re usle for the wvelength of 800 nm n less thn 0 % re usle for nm. Prtile types Numer spetr otine nm of t Numer of spetr otine t 800 nm for four ifferent lser energies 0. mj 0.3 mj.7 mj 3. mj 3.5 mj t F t F t F t F t F t F t F t F t F t F PSL PSL800 0 NA PSL0 0 NA Sili NCl NH NO AuAg Au Sili AuPAH

5 Tle S 3: Prtile smples use in this stuy. The smples mrke y n sterisk were originlly polyisperse, n sizeselete through DMA. m = eletril moility imeter; p= geometri imeter. Smple Venor Prtile imeter p (nm) PSL0 Thermo Sientifi, USA 0 PSL800 Thermo Sientifi, USA 800 PSL0 Thermo Sientifi, USA 0 NCl Merk KGA 00 NH NO 3 Merk KGA 00 SiO Pls AG 0 AuAg Nnoprtz In, USA 00 (300 nm ore n nm thik shell) AuPAH Nnoprtz In, USA 00 (300 nm ore n nm thik shell) AuSiO Nnoprtz In, USA 00 (300 nm ore n nm thik shell) 5 Bem imeter n power ensity lultions The lser em imeter t fous position is lulte y using the Eqution n for other positions lulte y Eqution. (Grf, 05) e f Dimeter t fous point = f = Eq. () Z Re (Z e f) Where e = initil em imeter f = fol length Z Re = Rleigh length efore the lens Z e = totl istne from soure to lens Dimeter t istne z from fous point = (z) = f z z R Eq. () 55 Spot size vrition ue to Spheril errtion= kd 3 /f Eq. (3) k = funtion of refrtive inex of the lens D = imeter of the em t fous f = fol length 0 The power ensities ting on the prtiles were lulte using the em imeters from tle S n the following eqution: Power ensity = energy per pulse pulse urtion em spot re Eq. () 5

6 Tle S : The lser em imeters for ifferent positions. 70 Lser Wvelength Bem Dimeter t Position F (μm) Bem Dimeter t Position F (μm) Bem Dimeter t Fous Position (μm) fslser 800 nm ±3 87±77 ±9 fslser nm 8±3 70±3 38±9 nslser 93 nm 8 ±7 99±3 37± Vriility of the totl ion intensity for onstnt onitions olleting 0 mss spetr Numer of spetr(#) 00 PSL_0nm_ with 8mJ pulse energy Suset () of this use for intensity versus power ensity omprision A Totl Ion Intensity 0 x 85 3 Figure S : Distriution of the numer of spetr otine for 0 nm PSL prtiles with the nslser t 8 mj energy for ifferent totl ion (oth positive n negtive) intensity. The spetr were selete from setion A shown in the plot. The Person's orreltion oeffiient is etween 0.7 n 0.9 for these selete spetr. 5

PSL 0 nm 00 Mesurement_ Mesurement_ 0 Intensity 800 00 00 00 0 8 TIme of Flight (ns) 8 0x Figure S 3: Reprouiility of spetr oserve with fslser for 0 nm PSL prtiles in two ifferent mesurements with

7 PSL 0 nm 00 Mesurement_ Mesurement_ 0 Intensity TIme of Flight (ns) 8 0x Figure S 3: Reprouiility of spetr oserve with fslser for 0 nm PSL prtiles in two ifferent mesurements with sme lser onitions (3. mj, 800 nm n sme fous position), the mesurement_ (re) n the mesurement_ (green) re the rw timeofflight spetr, these re the verge spetr of 0 prtiles. The spetrl fetures re nerly sme in ifferent mesurements, Person's orreltion oeffiient etween these spetr is ~0.9, n the remining reltively smll shift in the peks is ue to the ifferene in initil ion timings. 90 Figure S : Reprouiility of positive spetr oserve with fslser ltion for 0 ifferent single 0 nm PSL prtiles with 3. mj energy per pulse. An offset ws e to the intensity sle to llow for etter omprison. Person's orreltion oeffiient etween these spetr is ~0.0.9 for these spetr.

Intensity 95 Figure S 5: Reprouiility of negtive mss spetr oserve with fslser ltion for 0 ifferent single 0 nm PSL prtiles with 3. mj energy per pulse.

8 Intensity 95 Figure S 5: Reprouiility of negtive mss spetr oserve with fslser ltion for 0 ifferent single 0 nm PSL prtiles with 3. mj energy per pulse. An offset ws e to the intensity sle to llow for etter omprison. Person's orreltion oeffiient etween these spetr is ~0.0.9 for these spetr. SiO mss spetr SiO spetr 0 3. mj/pulse 0 3. mj/pulse Negtive mj/pulse mj/pulse Negtive 5 Timeofflight (ns) 0 5x 5 Timeofflight (ns) 0 5x Figure S : SiO rw spetr for ifferent lser energies for fslser ltion t 800 nm. () & () re positive n negtive spetr t 3. mj energy per pulse () & () re positive n negtive spetr t 0.3 mj energy per pulse. More lusters form t higher pulse energies. 7

9 Comprison of single prtile mss spetr otine using 93 nm (ns pules), nm (fs pulses), n 800 nm (fs pulses) The mss spetr for PSL prtiles of 0 nm imeter re shown in Fig. S7 n Fig. S7 with the only remrkle ifferene eing the reue verge ion intensity for nm. These spetr re similr to the type spetr (f. Fig. 3ef) otine using the fslser with 800 nm. The ATOFMS with nm nnoseon lser pulses genertes similr positive ion spetr (Gälli et l., 00) ut more spetrl signtures on the negtive ion spetr. For NCl erosol prtiles (f. Fig. S8), the nm fslaaptof results in the sme positive n negtive spetr s for 800 nm (f. Fig. ), n the mjor ifferenes oserve re less NO ions n less Cl peks in the negtive spetr for nm. N Cl, NCl lso exist in the positive spetrum. Crson et l. (997, 995) generte very similr single prtile mss spetr for NCl prtiles with 8 nm, 5 mj pulse energy, n.5 ns pulse urtion. However, the verge ion intensity is times smller thn with 800 nm fslser pulses. Ammonium nitrte prtiles (f. Fig. S9) ionize with nm fs pulses result in the sme positive (NO, NO, n NO ) ion spetrl fetures s when using 800 nm fs pulses (f. Fig. S9ef ), ut with no NH /O, OH, NH signture n less verge ion intensity n more negtive ion signtures. Brns et l. (0) oserve mjor peks for NO / /, NO, N, NO 3, n more positive lusters with nm ns pulses using n ATOFMS. Single prtile mss spetr for SiO prtiles re shown in Fig. S for ifferent esorption n ioniztion wvelengths. The mss spetr show very similr spetrl fetures in the negtive ion spetr for oth 800 nm n nm of the fslser, however, smller numer of Si xo y lusters is oserve in the fslser nm positive spetr. For nm the intensities re smller n hene the lrger ions less visile. Furthermore, the O ions re missing. Similr mss spetr were oserve when using nm ATOFMS for Silion rih prtiles with minly SiO n SiO signtures (Dll Osto et l., 00). For ll oreshell prtiles (f. Figs SS3), the spetrl signtures originting from itionl surfe otings e.g. y wter or the surftnt (Cetyltrimethylmmonium romie) re very similr when using fslser pulses of n 800 nm. No gol signtures were oserve for ny of the oreshell prtiles using nm n 800 nm fslser pulses, espite the lower refletivity of gol in the UV. Spener et l. (008) hve oserve surfe plsmon effets with nm nnoseon ATOFMS uring lser esorption n ionistion for gol nnoprtiles. They reporte very similr gol ion signtures s we hve oserve for 93 nm nslser pulses n silver ote gol prtiles. However, we oul not etet ny suh gol relte ion signtures with the fslser t nm or 800 nm. 8

10 Signl / mv Signl / mv C C C 3 C O O C O C C Ar CO C 3 C C 5 C 3 C Ar C C O C C 3 C C7 59 C 5 C 5 H C 5 H C 5 H C 5 C C 7 C8 C9 C C C C C C 5 C C 5 C 59 0 C 7 C 8 C 5 C 5 H C 5 H C 7 C 8 C9 H O C 3 5 C C e g C C 3 H C 3 C O H C C 3 Negtive C C C5 C C 7 C 8 Eximer93 nm FS nm FS800 nm f h Figure S 7: Bipolr mss spetr of single PSL prtiles of p= 0 nm. : Typil nslser spetr (93 nm); : fslser (λ = nm) spetr; ef: fslser (λ = 800 nm) spetr for 5 % of prtiles (type ); g h: fslser (λ = 800 nm) spetr for % of prtiles (type ). The pulse energy is mj for the nslser, 0. mj for fs nm, n 3. mj for the fs800 nm. N N N Cl N 3 Cl O N Cl Negtive NCl Eximer93 nm Fs nm FS800 nm N Cl N Cl N Cl 3 N O N N Cl Cl N Cl N 3 Cl (NCl) Cl H N e H NO Cl NO N N O Cl N Cl Cl NCl N 3 Cl N N N Cl _ 00 N Cl 3 00 f (NCl) 5 Figure S 8: Bipolr mss spetr of NCl single prtiles of m= 00 nm. : Typil nslser spetr (93 nm); : fslser (λ = nm) spetr. e f: fslser (λ = 800 nm) spetr. The pulse energy is mj for the nslser, 0. mj for fs nm, n 3. mj for the fs800 nm. 9

11 Signl / mv Signl / mv NO NO NH NH NO OH OH NO 3 NO NOO NH N N (NH ) NO (NH NO NO ) 3 N N NO (NH ) (NH ) 3 N NO Negtive NO 3 HNO 3 NO H N NH NO /O NH OH N (NH ) NO NO N O (NH ) 3 e H N N NO O NO Eximer93 nm FS nm FS800 nm f Figure S 9: Bipolr mss spetr of NHNO3 prtiles of p= 00 nm. : Typil nslaaptof spetr (93 nm); : fslaaptof (λ = nm) spetr. e f: fslser (λ = 800 nm) spetr. The pulse energy is mj for the nslser, 0. mj for fs nm, n 3. mj for the fs800 nm. SiO O 3 SiO Si Negtive O SiO SiO 3 Eximer93 nm FSUV nm FSIR800 nm Si SiO SiO 3 Si SiO SiO Si O 5 3 Si 3 O 7 Si SiO O O SiO SiO 3 Si O 3 Si O 5 Si 3 O 7 e SiO O SiO SiO 3 Si O 5 Si Si O Si 3 O 7 f Si O 9 Si 5 O Si O Figure S : Bipolr mss spetr of single SiO prtiles of p= 0 nm. : Typil nslser spetr (93 nm); : fslser (λ = nm) spetr; ef: fslser (λ = 800 nm) spetr. The pulse energy is mj for the nslser, 0. mj for fs nm, n 3. mj for the fs800 nm.

12 Signl / mv Signl / mv Surftnt Ag(7,9) Surftnt Au AuO Ag(7,9) Br AgO (39,) Ag(7,9) Br Surftnt Negtive Ag(7,9) Au Ag O 3 Surftnt Ag(7,9) Br AgO (39,) e Ag(7,9) Eximer93 nm FS nm FS800 nm f Figure S : Bipolr mss spetr of golsilver oreshell prtiles of p= 00 nm. : Typil ns LAAPTOF spetr (93 nm); : fslaaptof (λ = nm) spetr. e f: fslser (λ = 800 nm) spetr. The pulse energy is mj for the nslser, 0. mj for fs nm, n 3. mj for the fs800 nm. (C n /C n H )n= Au (C n /C n H )n=7 Negtive Au (C n /C n H /(CHN) n ) Au C 3 C C Eximer93 nm Fs nm FS800 nm (C n /C n H /(CHN) n ) Au e (CHN) n ) C f Figure S : Bipolr mss spetr of AuPAH oreshell prtiles. : Typil nslaaptof spetr (93 nm); : fslaaptof (λ = nm) spetrum tht ontins only PAH signl, ef: fslaaptof (λ=800nm) spetrum lso without gol signl. The pulse energy is mj for the nslser, 0. mj for fs C nm, n 3. mj for the fs800 nm.

13 Averge Ion Intensity (Signl/mv) Si Au O O SiO O C C 3 SiO SiO C SiO Negtive Au Signl / mv O OH Si SiO C 5 O SiO Si SiO C C 5 SiO Si SiO O C 5 SiO e Au Si O SiO C 5 Eximer93 nm FS nm FS800 nm Au f Figure S 3: Bipolr mss spetr of AuSiO oreshell prtiles. : Typil nslaaptof spetr (93 nm); : fslaaptof (λ = nm) spetrum tht ontins only SiO signl, ef: fslaaptof (λ=800nm) spetrum without gol signl. The pulse energy is mj for the nslser, 0. mj for fs nm, n 3. mj for the fs800 nm. 5 Vrition of totl verge ion intensity with vrition in the power ensity Nnoseon Femtoseon x Power Density (Wm ) x x PSL 0 nm PSL 0 nm AuAg 00 nm Sili 0 nm NCl 00 nm 5 5 Power Density (Wm ) 0x Figure S : Vrition of verge ion intensity for F n F position versus lser power ensity for ifferent prtile types. () () Eximer lser, n () () fslser, respetively. The power ensity of

14 70 the lser ting on the prtiles epens on the position of the fous reltive to the prtiles, n it will e higher (y ftor of ~.5) loser to fous postion (F) thn further wy from the fous (F). This orrespons to ifferene of ftor of for the verge ion intensities. Error rs enote ± stnr evition. 75 Referenes Hm, A. H.: High Energy n Short Pulse Lsers: Effets of Different Lser Pulse Regimes (Nnoseon, Pioseon n Femtoseon) on the Altion of Mterils for Proution of Nnoprtiles in Liqui Solution, 0. Royon, A., Petit, Y., Ppon, G., Rihrson, M., n Cnioni, L.: Femtoseon lser inue photohemistry in mterils tilore with photosensitive gents [Invite], Opt. Mter. Express,, 8 88, 0. Bulgkov, A. V., Ozerov, I., n Mrine, W.: Silion lusters proue y femtoseon lser ltion: nontherml emission n gsphse onenstion, Applie Physis A, 79, 5959, 00. Grf, T.: Lser Grunlgen er Lserstrhlerzeugung. Springer Vieweg, 05. Hrill, S. S., Freemn, J. R., Diwkr, P. K., n Hssnein, A.: Femtoseon Lser Altion: Funmentls n Applitions. In: LserInue Brekown Spetrosopy: Theory n Applitions, Muszzi, S. n Perini, U. (Es.), Springer Berlin Heielerg, Berlin, Heielerg, 0. Kto, T., Koyshi, T., Mtsuo, Y., KurtNishimur, M., Oym, R., Mtsumur, Y., Ymmoto, H., Kwi, J., n Hyshizki, Y.: Comprison etween femtoseon n nnoseon lser ltion of solution smples pplie on sustrte, Journl of Physis: Conferene Series, 59, 37, 007. Murphy, D. M. n Thomson, D. S.: Lser Ioniztion Mss Spetrosopy of Single Aerosol Prtiles, Aerosol Siene n Tehnology,, 379, 995. Royon, A., Petit, Y., Ppon, G., Rihrson, M., n Cnioni, L.: Femtoseon lser inue photohemistry in mterils tilore with photosensitive gents [Invite], Opt. Mter. Express,, 8 88, 0. Zwowiz, M. A., Aelmonem, A., Mohr, C., Sthoff, H., Froy, K. D., Murphy, D. M., Leisner, T., n Czizo, D. J.: SinglePrtile TimeofFlight Mss Spetrometry Utilizing Femtoseon Desorption n Ioniztion Lser, Anlytil Chemistry, 87, 9, 05. Zhou, L., Prk, K., Milherg, H. M., n Zhrih, M. R.: Unerstning the Intertion of n Intense Lser Pulse with Nnoprtiles: Applition to the Quntifition of Single Prtile Mss Spetrometry, Aerosol Siene n Tehnology,, 8887, Gälli, M., Guzzotti, S. A., n Prther, K. A.: Improve Lower Prtile Size Limit for Aerosol TimeofFlight Mss Spetrometry, Aerosol Siene n Tehnology, 3, 38385, 00. Crson, P. G., Johnston, M. V., n Wexler, A. S.: RelTime Monitoring of the Surfe n Totl Composition of Aerosol Prtiles, Aerosol Siene n Tehnology,, 9300, 997. Crson, P. G., Neuuer, K. R., Johnston, M. V., n Wexler, A. S.: Online hemil nlysis of erosols y rpi singleprtile mss spetrometry, Journl of Aerosol Siene,, 53555, 995. Brns, M., Kmphus, M., Böttger, T., Shneier, J., Drewnik, F., Roth, A., Curtius, J., Voigt, C., Boron, A., Beekmnn, M., Bouron, A., Perrin, T., n Borrmnn, S.: Chrteriztion of Newly Develope AirrftBse Lser Altion Aerosol Mss Spetrometer (ALABAMA) n First Fiel 3

15 0 Deployment in Urn Pollution Plumes over Pris During MEGAPOLI 009, Aerosol Siene n Tehnology, 5,, 0. Dll Osto, M., Beows, D. C. S., Kinnersley, R. P., Hrrison, R. M., Donovn, R. J., n Hel, M. R.: Chrteriztion of iniviul irorne prtiles y using erosol timeofflight mss spetrometry t Me He, Ireln, J. Geophys. Res.Atmos., 9, D30, Spener, M. T., Furutni, H., Olenurg, S. J., Drlington, T. K., n Prther, K. A.: Gol Nnoprtiles s Mtrix for VisileWvelength SinglePrtile MtrixAssiste Lser Desorption/Ioniztion Mss Spetrometry of Smll Biomoleules, The Journl of Physil Chemistry C,, , 008.

Particle Physics. Michaelmas Term 2011 Prof Mark Thomson. Handout 3 : Interaction by Particle Exchange and QED. Recap

Particle Physics. Michaelmas Term 2011 Prof Mark Thomson. Handout 3 : Interaction by Particle Exchange and QED. Recap Prtile Physis Mihelms Term 2011 Prof Mrk Thomson g X g X g g Hnout 3 : Intertion y Prtile Exhnge n QED Prof. M.A. Thomson Mihelms 2011 101 Rep Working towrs proper lultion of ey n sttering proesses lnitilly