Investigation of the laser fluence and wavelength dependence in surface-assisted laser desorption/ionization mass spectrometry using gold nanoparticles.

IF 1.8 3区 化学 Q4 BIOCHEMICAL RESEARCH METHODS Rapid Communications in Mass Spectrometry Pub Date : 2024-08-31 DOI:10.1002/rcm.9895
Wendy H Müller, Alexander Potthoff, Klaus Dreisewerd, Jens Soltwisch
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Abstract

Rationale: Surface-assisted laser desorption/ionization (SALDI) mass spectrometry (MS) builds on the use of nanostructured surfaces (e.g., coatings of colloidal nanoparticles) to promote analyte desorption and ionization. The SALDI process is believed to occur mainly through thermal processes, resulting from heating of the nanosubstrate upon absorption of the photon energy, and by assisting ionization steps. Mostly due to the accessibility of the respective hardware, the majority of SALDI-MS studies use standard laser wavelengths for MALDI (i.e., 337 or 355 nm), even though peak absorption of the SALDI nanosubstrate might completely differ from these values.

Methods: Here, we investigated the wavelength dependence in SALDI-MS to determine if wavelength adjustment would be beneficial, and to provide new experimental data for a better understanding of the SALDI mechanism. To this end, gold nanoparticles (AuNPs) sprayed onto microscope glass slides were employed as SALDI nanosubstrates and L-arginine as a model analyte. In addition, we used 2,5-dihydroxyacetophenone (2,5-DHAP) for classical MALDI-MS using the same experimental setup. Arginine ion signals were recorded as a function of laser wavelength and laser fluence. Mass spectra were acquired in the wavelength range between 310 and 630 nm, including the absorption maximum of the sprayed AuNPs around 550 nm and that of 2,5-DHAP around 380 nm.

Results: Laser fluence thresholds for the generation of arginine ions were found to be dependent on the laser wavelength and to inversely correlate with the absorbance profiles of the deposited AuNPs and 2,5-DHAP, respectively. Very differently to MALDI, in SALDI ionization efficiency was found to strictly linearly decrease with increasing laser wavelength.

Conclusions: Our results, therefore, corroborate the general assumption that material ejection in SALDI-MS is mainly driven by thermal processes in the low laser fluence range and add new evidence that the ionization process is directly influenced by photon energy when AuNPs are employed as nanosubstrates.

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利用金纳米粒子研究表面辅助激光解吸电离质谱法中的激光通量和波长依赖性。
原理:表面辅助激光解吸/电离(SALDI)质谱(MS)是利用纳米结构表面(如胶体纳米粒子涂层)来促进分析物的解吸和电离。据信,SALDI 过程主要是通过热过程(纳米基底吸收光子能量后受热)和辅助电离步骤实现的。方法:在此,我们研究了 SALDI-MS 的波长依赖性,以确定调整波长是否有益,并为更好地理解 SALDI 机制提供新的实验数据。为此,我们采用喷涂在显微镜玻璃载玻片上的金纳米粒子(AuNPs)作为 SALDI 纳米基底,并以 L-精氨酸作为模型分析物。此外,我们还使用相同的实验装置,将 2,5-二羟基苯乙酮(2,5-DHAP)用于经典的 MALDI-MS。精氨酸离子信号记录为激光波长和激光能量的函数。质谱采集的波长范围为 310 至 630 nm,其中包括喷涂 AuNPs 在 550 nm 附近的吸收最大值和 2,5-DHAP 在 380 nm 附近的吸收最大值:结果:发现生成精氨酸离子的激光通量阈值取决于激光波长,并分别与沉积的 AuNPs 和 2,5-DHAP 的吸光度曲线成反比。与 MALDI 非常不同的是,SALDI 电离效率随着激光波长的增加呈严格的线性下降趋势:因此,我们的研究结果证实了 SALDI-MS 中的物质喷射主要由低激光通量范围内的热过程驱动的一般假设,并为采用 AuNPs 作为纳米基质时离子化过程直接受光子能量影响提供了新的证据。
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来源期刊
CiteScore
4.10
自引率
5.00%
发文量
219
审稿时长
2.6 months
期刊介绍: Rapid Communications in Mass Spectrometry is a journal whose aim is the rapid publication of original research results and ideas on all aspects of the science of gas-phase ions; it covers all the associated scientific disciplines. There is no formal limit on paper length ("rapid" is not synonymous with "brief"), but papers should be of a length that is commensurate with the importance and complexity of the results being reported. Contributions may be theoretical or practical in nature; they may deal with methods, techniques and applications, or with the interpretation of results; they may cover any area in science that depends directly on measurements made upon gaseous ions or that is associated with such measurements.
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