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Title 

Expansion cooling in the matrix plume is under-recognized in MALDI mass spectrometry

Authors 

Y J BaeJeong Hee MoonM S Kim

Publisher 

Elsevier

Issue Date 

2011

Citation 

Journal of American Society for Mass Spectrometry, vol. 22, no. 6, pp. 1070-1078

Keywords 

Dissociation efficiencyExpansion coolingIn-source decayMALDIPeptide dissociationPlume temperaturePost-source decay

Abstract 

Time-of-flight (TOF) mass spectra for a peptide (Y6) were obtained by utilizing matrix-assisted infrared laser desorption ionization (IR-MALDI) with glycerol as the matrix and by ultraviolet MALDI with α-cyano-4-hydroxycinnamic acid (CHCA), sinapinic acid (SA), and 2,5-dihydroxybenzoic acid (DHB). Collisional activation during ion extraction and exothermicity in the gas-phase proton transfer were found to be unimportant as the driving forces for in-source (ISD) and post-source (PSD) decays, indicating that the thermal energy acquired during photo-ablation is responsible for their occurrence. The temperatures of [Y6∈+∈H] + in the 'early' and 'late' matrix plumes were estimated by the kinetic analysis of the ISD and PSD yields, respectively. The order of the temperatures was glycerol∈<∈DHB∈?∈SA∈<∈ CHCA in the early plume and glycerol∈<∈DHB∈<∈SA∈ <∈CHCA in the late plume. For each matrix, the temperature in the late plume was lower than in the early plume by 300-400 K, which was attributed to expansion cooling. The model (thermalization followed by expansion cooling) proposed to explain the occurrence of both rapid ISD and slow PSD is not only in sharp contrast with but also mutually exclusive with the prevailing explanation that the exothermicity in proton transfer and in-plume collisional activation are the driving forces for ion fragmentation in MALDI. The model also explains why MALDI is more successful for mass spectrometry of labile molecules than other desorption techniques that do not utilize a matrix. Factors affecting the plume temperature are also discussed.

ISSN 

1044-0305

Link 

http://dx.doi.org/10.1007/s13361-011-0115-y

Appears in Collections

1. Journal Articles > Journal Articles

Registered Date

2017-04-19


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