Wavelength-selective laser desorption of doped ice surfaces

Mihesan, C.; Ziskind, Michaël; Chazallon, Bertrand; Therssen, E.; Desgroux, Pascale; Focşa, Cristian

doi:10.1016/j.susc.2005.06.064

Cited by 9 publications

(24 citation statements)

References 20 publications

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“…3 Unlike in MALDI mass spectrometry, where a single laser pulse is used for both matrix ablation and analyte ionization, our method utilizes an infrared (IR) laser that resonantly ex- cites H 2 O vibrations leading to the ablation of the ice matrix, followed by an ultraviolet (UV) laser to ionize ablated species through resonant multiphoton ionization, and subsequent time-of-flight (TOF) mass spectroscopic analysis of the ionized species. The present method, though not as common as the UV-MALDI or IR-MALDI, 2,4 has been shown to be effective in investigating ices by other researchers as well, 5,6 but our recent publication 3 is the first to show that chemical reaction pathways in cryogenic ices can be investigated by this method. We have demonstrated that when polycyclic aromatic hydrocarbons (PAHs) imbedded in water-ice were photolyzed with vacuum ultraviolet (VUV) hydrogen lamp (121.6 nm Ly α hydrogen line), these molecules undergo hydrogenation and hydroxylation even at temperatures as low as 5 K.…”

Section: Introductionmentioning

confidence: 81%

Novel two-step laser ablation and ionization mass spectrometry (2S-LAIMS) of actor-spectator ice layers: Probing chemical composition of D2O ice beneath a H2O ice layer

Yang

Gudipati

2014

The Journal of Chemical Physics

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In this work, we report for the first time successful analysis of organic aromatic analytes imbedded in D2O ices by novel infrared (IR) laser ablation of a layered non-absorbing D2O ice (spectator) containing the analytes and an ablation-active IR-absorbing H2O ice layer (actor) without the analyte. With these studies we have opened up a new method for the in situ analysis of solids containing analytes when covered with an IR laser-absorbing layer that can be resonantly ablated. This soft ejection method takes advantage of the tenability of two-step infrared laser ablation and ultraviolet laser ionization mass spectrometry, previously demonstrated in this lab to study chemical reactions of polycyclic aromatic hydrocarbons (PAHs) in cryogenic ices. The IR laser pulse tuned to resonantly excite only the upper H2O ice layer (actor) generates a shockwave upon impact. This shockwave penetrates the lower analyte-containing D2O ice layer (spectator, a non-absorbing ice that cannot be ablated directly with the wavelength of the IR laser employed) and is reflected back, ejecting the contents of the D2O layer into the vacuum where they are intersected by a UV laser for ionization and detection by a time-of-flight mass spectrometer. Thus, energy is transmitted from the laser-absorbing actor layer into the non-absorbing spectator layer resulting its ablation. We found that isotope cross-contamination between layers was negligible. We also did not see any evidence for thermal or collisional chemistry of PAH molecules with H2O molecules in the shockwave. We call this "shockwave mediated surface resonance enhanced subsurface ablation" technique as "two-step laser ablation and ionization mass spectrometry of actor-spectator ice layers." This method has its roots in the well-established MALDI (matrix assisted laser desorption and ionization) method. Our method offers more flexibility to optimize both the processes--ablation and ionization. This new technique can thus be potentially employed to undertake in situ analysis of materials imbedded in diverse media, such as cryogenic ices, biological samples, tissues, minerals, etc., by covered with an IR-absorbing laser ablation medium and study the chemical composition and reaction pathways of the analyte in its natural surroundings.

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Section: Introductionmentioning

confidence: 81%

Novel two-step laser ablation and ionization mass spectrometry (2S-LAIMS) of actor-spectator ice layers: Probing chemical composition of D2O ice beneath a H2O ice layer

Yang

Gudipati

2014

The Journal of Chemical Physics

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“…The experimental set-up has been extensively detailed in previous papers [10][11][12][13][14][15]. Briefly, our approach is based on the coupling of three techniques:…”

Section: Methodsmentioning

confidence: 99%

“…However, Haefliger and Zenobi demonstrated that single wavelength, two photon REMPI is not very selective for desorbed PAH because of the high temperature of the PAH gas [17]. Variation of the wavelength and fluence of the desorption laser for selective desorption of PAH isomers from solid PAH samples has been suggested by Focsa et al [10,11,14,15]. An entirely different approach is the use of very high fluence ionization laser pulses to ionize the desorbed PAH and to use the fragmentation patterns to resolve the isomers present in the desorbed plume [20][21][22].…”

Section: Evolution Of the Mass Spectra With The Ionization Fluence: Smentioning

confidence: 99%

Influence of the photoionization process on the fragmentation of laser desorbed polycyclic aromatic hydrocarbons

Thomson

Ziskind

Mihesan

et al. 2007

Applied Surface Science

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“…Indeed, recently a number of new developments have been reported. [22][23][24][25][26][27][28][29][30][31][32] Successful experiments have been reported in which TPD has been combined with vacuum UV (VUV) single photo-ionisation time-of-flight mass spectrometry (TOF-MS), measuring the mass from desorbing species from the ice. 22,23 Diagnostic techniques such as Substrate/Matrix Assisted Laser Desorption Ionisation Time-ofFlight Mass Spectrometry ((S/M)ALDI-TOF-MS) have been introduced.…”

Section: Introductionmentioning

confidence: 99%

Laser desorption time-of-flight mass spectrometry of ultraviolet photo-processed ices

Paardekooper

Bossa

Isokoski

et al. 2014

Review of Scientific Instruments

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A new ultra-high vacuum experiment is described that allows studying photo-induced chemical processes in interstellar ice analogues. MATRI(2)CES - a Mass Analytical Tool to study Reactions in Interstellar ICES applies a new concept by combining laser desorption and time-of-flight mass spectrometry with the ultimate goal to characterize in situ and in real time the solid state evolution of organic compounds upon UV photolysis for astronomically relevant ice mixtures and temperatures. The performance of the experimental setup is demonstrated by the kinetic analysis of the different photoproducts of pure methane (CH4) ice at 20 K. A quantitative approach provides formation yields of several new species with up to four carbon atoms. Convincing evidence is found for the formation of even larger species. Typical mass resolutions obtained range from M/ΔM ∼320 to ∼400 for CH4 and argon, respectively. Additional tests show that the typical detection limit (in monolayers) is ⩽0.02 ML, substantially more sensitive than the regular techniques used to investigate chemical processes in interstellar ices.

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Wavelength-selective laser desorption of doped ice surfaces

Cited by 9 publications

References 20 publications

Novel two-step laser ablation and ionization mass spectrometry (2S-LAIMS) of actor-spectator ice layers: Probing chemical composition of D2O ice beneath a H2O ice layer

Novel two-step laser ablation and ionization mass spectrometry (2S-LAIMS) of actor-spectator ice layers: Probing chemical composition of D2O ice beneath a H2O ice layer

Influence of the photoionization process on the fragmentation of laser desorbed polycyclic aromatic hydrocarbons

Laser desorption time-of-flight mass spectrometry of ultraviolet photo-processed ices

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