Reproducibility of Temperature-Selected Mass Spectra in Matrix-Assisted Laser Desorption Ionization of Peptides

Bae, Yong Jin; Park, Kyung Man; Kim, Myoung Soo

doi:10.1021/ac3014077

Cited by 38 publications

(75 citation statements)

References 34 publications

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“…We took the temperature in the early plume (T early ) [12] where in-source decay [13] occurred as the representative temperature of each MALDI event. We then found that the observed spectral changes were correlated with the lowering of T early as the sample became thinner upon repetitive irradiation [10]. 2.…”

Section: Introductionmentioning

confidence: 82%

“…The vacuum-drying of such a solution is known to produce a rather homogeneous solid sample [10,11]. When we repetitively irradiated a spot on such a sample with laser pulses, we observed that the abundance of each ion appearing in the mass spectrum, both analyteand matrix-derived, changed systematically.…”

Section: Introductionmentioning

confidence: 98%

“…3. When T early was fixed, we found that the reaction quotient (Q) for the matrix-to-analyte proton transfer, reaction 1, was nearly constant [10,16].…”

Section: Introductionmentioning

confidence: 98%

“…Recently, we studied MALDI for solid samples prepared from solutions containing peptides (analytes) and α-cyano-4-hydroxycinnamic acid (CHCA, matrix) [10]. The vacuum-drying of such a solution is known to produce a rather homogeneous solid sample [10,11].…”

Section: Introductionmentioning

confidence: 99%

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Investigations of Some Liquid Matrixes for Analyte Quantification by MALDI

Moon

Park

Ahn

et al. 2015

J. Am. Soc. Mass Spectrom.

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Abstract. Sample inhomogeneity is one of the obstacles preventing the generation of reproducible mass spectra by MALDI and to their use for the purpose of analyte quantification. As a potential solution to this problem, we investigated MALDI with some liquid matrixes prepared by nonstoichiometric mixing of acids and bases. Out of 27 combinations of acids and bases, liquid matrixes could be produced from seven. When the overall spectral features were considered, two liquid matrixes using α-cyano-4-hydroxycinnamic acid as the acid and 3-aminoquinoline and N,N-diethylaniline as bases were the best choices. In our previous study of MALDI with solid matrixes, we found that three requirements had to be met for the generation of reproducible spectra and for analyte quantification: (1) controlling the temperature by fixing the total ion count, (2) plotting the analyte-to-matrix ion ratio versus the analyte concentration as the calibration curve, and (3) keeping the matrix suppression below a critical value. We found that the same requirements had to be met in MALDI with liquid matrixes as well. In particular, although the liquid matrixes tested here were homogeneous, they failed to display spot-to-spot spectral reproducibility unless the first requirement above was met. We also found that analytederived ions could not be produced efficiently by MALDI with the above liquid matrixes unless the analyte was sufficiently basic. In this sense, MALDI processes with solid and liquid matrixes should be regarded as complementary techniques rather than as competing ones.

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Section: Introductionmentioning

confidence: 82%

Section: Introductionmentioning

confidence: 98%

“…3. When T early was fixed, we found that the reaction quotient (Q) for the matrix-to-analyte proton transfer, reaction 1, was nearly constant [10,16].…”

Section: Introductionmentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

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Investigations of Some Liquid Matrixes for Analyte Quantification by MALDI

Moon

Park

Ahn

et al. 2015

J. Am. Soc. Mass Spectrom.

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“…4,5 In contrast, in the second group, photo-excitation is simply an instantaneous way of supplying thermal energy to the sample and hence inducing its ablation. [6][7][8][9] The thermal energy needed for ablation is supplied by photo-excitation in the first group of hypotheses also. Ionization of matrix molecules via pooling of excitons is the leading hypothesis belonging to the first group, while thermal processes such as the pre-formed ion emission have been proposed for the second group.…”

Section: Matrix-assisted Laser Desorption Ionization (Maldi)mentioning

confidence: 99%

Efficiency of Gas-Phase Ion Formation in Matrix-Assisted Laser Desorption Ionization with 2,5-Dihydroxybenzoic Acid as Matrix

Park¹,

Ahn²,

Bae³

et al. 2013

Bulletin of the Korean Chemical Society

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Numbers of matrix-and analyte-derived ions and their sum in matrix-assisted laser desorption ionization (MALDI) of a peptide were measured using 2,5-dihydroxybenzoic acid (DHB) as matrix. As for MALDI with α-cyano-4-hydroxy cinnamic acid as matrix, the sum was independent of the peptide concentration in the solid sample, or was the same as that of pure DHB. This suggested that the matrix ion was the primary ion and that the peptide ion was generated by matrix-to-peptide proton transfer. Experimental ionization efficiencies of 10 -10 −3 for matrices speculated by Hillenkamp and Karas. Number of gas-phase ions generated by MALDI was unaffected by laser wavelength or pulse energy. This suggests that the main role of photo-absorption in MALDI is not in generating ions via a multi-photon process but in ablating materials in a solid sample to the gas phase.

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Preparation of Homogeneous Solid Samples for Reproducible and Quantitative MALDI

Ahn

Park

Moon

et al. 2016

Bulletin Korean Chem Soc

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Preparing samples with good homogeneity is one of the requirements for generating reproducible matrix‐assisted laser desorption ionization (MALDI) spectra and for using them in analyte quantification. Thus far, we have not been successful in producing homogeneous solid samples from popular matrixes apart from α‐cyano‐4‐hydroxycinnamic acid (CHCA). In this work, we demonstrate the production of an outwardly homogeneous solid sample by loading a methanol solution of a matrix into a shallow reservoir on a coated MALDI sample plate and then vacuum‐drying it. Out of ten popular matrixes tested, seven yielded homogeneous samples. These were 9‐aminoacridine, 6‐aza‐2‐thiothymine, CHCA, 2,5‐dihydroxybenzoic acid, ferulic acid, sinapinic acid, and 2,4,6‐trihydroxyacetophenone. For MALDI with these matrixes, linear calibration curves covering wide dynamic ranges were acquired. Performances of these matrixes in various aspects of analyte quantification have been investigated.

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Reproducibility of Temperature-Selected Mass Spectra in Matrix-Assisted Laser Desorption Ionization of Peptides

Cited by 38 publications

References 34 publications

Investigations of Some Liquid Matrixes for Analyte Quantification by MALDI

Investigations of Some Liquid Matrixes for Analyte Quantification by MALDI

Efficiency of Gas-Phase Ion Formation in Matrix-Assisted Laser Desorption Ionization with 2,5-Dihydroxybenzoic Acid as Matrix

Preparation of Homogeneous Solid Samples for Reproducible and Quantitative MALDI

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