NanoSIMS Techniques and Its Important Implications in Geomicrobiology and Biosedimentology
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摘要: 纳米离子探针（NanoSIMS）技术具有高空间分辨率和高化学灵敏度的特点，是目前国际上最先进的原位微区分析手段之一.它能在纳米尺度上进行元素和同位素分布的原位分析，为揭示微生物与环境的相互作用提供了革命性技术；因此在地质微生物学和生物沉积学研究中展现出重要应用潜力甚至在某些方向的研究中不可或缺.本文在介绍NanoSIMS的工作原理基础上，综述了NanoSIMS技术在地质微生物学领域最前沿的重要应用，重点解剖其在现代微生物群落功能研究、深时碳酸盐矿物沉淀、生物地球化学循环、地球早期生命信号的识别以及地外生命探索等方面的应用实例.总之，NanoSIMS技术的发展与应用推动了地质微生物学研究迈向更高空间分辨率的微观世界，为探索地球生命起源和地外星球宜居性提供了前所未有的机遇.同时，本文论述了NanoSIMS在样品制备、信噪比、定量分析等方面的挑战，并展望了该技术优化方向，如技术升级、多技术联用和算法改进等，希望为多学科原位微区分析提供重要技术支撑，并进一步推动地质微生物学和生物沉积学及相关交叉学科的发展.Abstract: NanoSIMS (nanoscale secondary ion mass spectrometry) technology, with its high spatial resolution and chemical sensitivity, demonstrates significant potential for implications in researches of geomicrobiology. This technology enables in-situ analysis of elemental and isotopic distributions at the nanoscale, offering a revolutionary tool for uncovering interactions between microorganisms and their environments. This article reviews the applications and advancements of NanoSIMS technology in the field of geomicrobiology. It provides a detailed overview of the principles of NanoSIMS and its applications in areas such as identifying biogenic minerals from ancient microorganisms, exploring extraterrestrial life, carbonate mineral precipitation, biogeochemical cycles, and functional studies of modern microbial communities. The development of NanoSIMS has propelled geomicrobiology towards greater precision and resolution, presenting unprecedented opportunities to study the origin of life, microbial activity in extreme environments, and global biogeochemical cycles. At the same time, this article identifies challenges related to sample preparation, signal-to-noise ratio, and quantitative analysis, while also suggesting directions for optimization, such as technological upgrades, multi-technique integration, and algorithmic improvements. In the future, the continued evolution of NanoSIMS will provide critical support for investigating early life on Earth, global elemental cycles, and extraterrestrial life, further advancing geomicrobiology and its related interdisciplinary fields.
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图 1 CAMECA NanoSIMS 50L型纳米离子探针设备（a）及其结构示意简图（b）
设备来自中国地质大学（武汉）地质微生物与环境全国重点实验室
Fig. 1. NanoSIMS (CAMECA NanoSIMS 50L) instrument (a) and the schematic diagram of the NanoSIMS 50L (b)
图 3 常见原位分析技术的空间分辨率和探测范围
SEM.扫描电镜；FE-SEM.场发射扫描电镜；TEM.透射电镜；FTIR.傅里叶变换红外光谱；Raman.拉曼光谱；EPMA.电子探针；LA-Q-ICPMS.激光剥蚀‒四级杆等离子体质谱；LA-MC-ICPMS.激光剥蚀‒多接收器等离子体质谱；LG-SIMS.大型离子探针；NanoSIMS.纳米离子探针；TOF-SIMS.飞行时间二次离子质谱离子探针；APT.三维原子探针.修改自Li and Li（2016）
Fig. 3. Spatial resolutions and detection ranges for common in-situ analysis techniques
图 5 太古代Farrel石英岩中一个大球体的NanoSIMS元素分布图
a~e. NanoSIMS元素分布碳（12C‒）、氮（12C14N‒）、硫（32S‒）、氧（16O‒）以及硅（28Si‒），离子强度的变化由校准条显示，颜色越亮表示强度越高；f. 球体在透射光下的光学显微照片；白色箭头指的是具有较高的12C‒、12C14N‒、32S‒；a~f中比例尺一致；图片来源于Oehler et al.（2010）
Fig. 5. NanoSIMS element maps of a large spheroid in chert from the Farrel quartzite
图 6 Tissint火星陨石中熔脉里面有机碳碳颗粒NanoSIMS成像
分析包括碳（C）、氢（12C1H-）、氮（12C14N-）、硫（S）、氯（Cl），离子强度的变化由校准条显示，颜色越亮表示强度越高.图片来源于Lin et al.（2014）
Fig. 6. NanoSIMS ion maps of organic carbons entrained in shock-melt veins of the Tissint meteorolite
图 7 现代微生物岩中丝状蓝藻的NanoSIMS离子图像
图中显示碳（12C-）、氮（26CN-）、硫（32S-）、氧（16O-）、镁（24Mg+）、钙（40Ca+）和硅（28Si-）的分布，以及扫描电镜电子图像（SE）.图像展示鞘（sheath）的纵向截面，鞘外被胞外聚合物（EPS）包围（在26CN-图像中由虚线圈出的亮区表示）.离子强度的变化由校准条显示，颜色越亮表示强度越高.文石颗粒与EPS紧密关联.比例尺为20 μm.图片来源于Wacey et al.（2010）
Fig. 7. NanoSIMS ion images of the filamentous cyanobacterium
图 8 西澳大利亚约27亿年前Tumbiana组微生物岩的NanoSIMS离子图像
图中展示碳（12C-）、氮（26CN-）、硫（32S-）、氧（16O-）、镁（24Mg+）、钙（40Ca+）和硅（28Si-）的分布.左上角为微生物岩的野外照片.样品中未发现微化石，但离子图像（12C-、26CN-和32S-，以及与16O-的反相关）突显贯穿图像中心和底部的有机物（在26CN-图像中用箭头标出）.离子强度的变化通过校准条表示，颜色越亮表示强度越高.此外，图像中同时存在碳酸钙和硅质颗粒，中心部分出现有机物可能捕获碳酸盐颗粒的现象（在40Ca+图像中用圆圈标出）.离子图像的比例尺为10 μm；野外照片中铅笔的长度为15 cm.图片来源于Wacey et al.（2010）
Fig. 8. NanoSIMS ion images of a microbialite from the ∼2 720 Ma Tumbiana Formation, Western Australia
图 9 单个细胞对碳（H13CO3‒）和氮（15NH4+）的吸收平行二次离子图像(a~c)，以及C. clathratiforme, L. purpurea, and C. okenii单个微生物细胞代谢活动中对碳和铵的吸收定量统计(d)
a（A~H）主要为C. clathratiforme细胞，b（A~D）主要为L. purpurea细胞，c（A~H）主要为C. okenii细胞.Cc代表C. clathratiforme，Lp代表L. purpurea，Co代表C. okenii，Nid代表未鉴定微生物，Agg代表为未鉴定的细菌的集合体，比例尺5 μm；d（A）中该线代表Redfield理论中海洋浮游植物的碳氮比约为6.6，并对总铵的贡献，d（B）为对总铵的贡献，d（C）为每个族群对系统中总溶解无机碳吸收的贡献.修改自Musat et al.（2008）
Fig. 9. Parallel secondary ion images of 15N-ammonium and 13C-inorganic carbon uptake by individual microorganism cells (a~c), and ammonium versus inorganic carbon uptake by individual C. clathratiforme, L. purpurea, and C. okenii cells (d)
图 10 利用同位素标记的13C碳酸氢盐（bicarbonate）和15N亮氨酸（leucine）培养的微生物细胞中13C和15N同位素富集的对比（a），浮游植物细胞与附着的细菌细胞的13C掺入率之间呈正相关（b-A），细菌与附着的浮游植物细胞的15N掺入率之间呈正相关（b-B）.修改自Arandia-Gorostidi et al. (2017)
图a中虚线为同位素天然丰度，每个点代表一个微生物细胞，通过整合NanoSIMS图像中定义的感兴趣区域的像素获得富集程度.NanoSIMS富集程度图像显示已鉴定的异养生物（Heterotrophs）和一个自养生物（Autotroph，白色箭头所指）
Fig. 10. Comparison between 13C and 15N isotopic enrichment for all analyzed microbial cells incubated with 13C bicarbonate and 15N leucine (a). Positive correlation between the 13C incorporation rates of phytoplankton cells and those of their attached bacterial cells, analyzed with a smaller raster for one of the replicates of the warm incubations (b-A), Similar positive correlation between the 15N incorporation rates of bacteria and those of the phytoplankton cells to which they were attached (b-B). Modified by Arandia-Gorostidi et al. (2017)
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