Takamizawa Atsushi, Fujimaki Susumu, Sunner Jan, Hiraoka Kenzo
Clean Energy Research Center, University of Yamanashi, Takeda 4-3-11, Kofu 400-8511, Japan.
J Am Soc Mass Spectrom. 2005 Jun;16(6):860-8. doi: 10.1016/j.jasms.2005.02.012. Epub 2005 Mar 29.
In laser spray, the tip of an electrospray capillary is irradiated with a continuous CO(2) laser beam. Here, we report results from a modified laser spray method that employs a relatively low laser irradiance level. With a laser power of approximately 2 W and a focal spot size ( approximately 0.3 mm), which covered the entire front surface of the electrospray capillary, the irradiance was approximately 3 x 10(3) W/cm(2). This resulted in a quiescent and smooth vaporization of aqueous solutions. This "evaporation-mode" laser spray method yielded the best results so far obtained in our laboratory with laser-irradiated electrospray, producing higher and more stable signals. The method was applied to the analysis of aqueous solutions of lysozyme and myoglobin. Mass spectra were obtained as a function of laser power from 0 W (electrospray) to approximately 2 W. The spray generated at the tip of the stainless steel capillary was observed with a CCD camera. With increase of laser power, the droplets in the spray became finer and the Taylor cone became progressively smaller. The strongest ion signals were recorded when the sample solution protruded only slightly from the tip of the capillary. A broadening of the lysozyme charge-state distribution, attributable to protein unfolding, was observed with a laser power of 2 W. No denaturation of myoglobin took place up to a laser power of 1.6 W. However, a sudden onset of denaturation was observed at 1.8 W as a broadening of the myoglobin charge distribution and the appearance of apo-myoglobin peaks. These findings demonstrate that laser spray is capable of dissociating the noncovalent complexes selectively without breaking covalent bonds.
在激光喷雾中,电喷雾毛细管的尖端用连续的CO₂激光束照射。在此,我们报告一种改进的激光喷雾方法的结果,该方法采用相对较低的激光辐照水平。激光功率约为2W,焦点尺寸(约0.3mm)覆盖电喷雾毛细管的整个前表面,辐照度约为3×10³W/cm²。这导致水溶液安静且平稳地蒸发。这种“蒸发模式”激光喷雾方法在我们实验室的激光辐照电喷雾中产生了迄今为止最好的结果,产生了更高且更稳定的信号。该方法应用于溶菌酶和肌红蛋白水溶液的分析。获得了从0W(电喷雾)到约2W的激光功率范围内的质谱。用CCD相机观察不锈钢毛细管尖端产生的喷雾。随着激光功率的增加,喷雾中的液滴变得更细,泰勒锥逐渐变小。当样品溶液仅从毛细管尖端略微突出时,记录到最强的离子信号。在2W的激光功率下,观察到溶菌酶电荷态分布变宽,这归因于蛋白质展开。在高达1.6W的激光功率下,肌红蛋白未发生变性。然而,在1.8W时观察到突然发生变性,表现为肌红蛋白电荷分布变宽和脱辅基肌红蛋白峰的出现。这些发现表明激光喷雾能够选择性地解离非共价复合物而不破坏共价键。