Solid immersion facilitates fluorescence microscopy with nanometer resolution and sub-ångström emitter localization.

Solid immersion facilitates fluorescence microscopy with nanometer resolution and sub-ångström emitter localization.
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DOI:
10.1002/adma.201203033
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发表时间:
2012-11-20
期刊:
影响因子:
29.4
通讯作者:
Smith, Jason M.
Smith, Jason M.
中科院分区:
材料科学1区
文献类型:
--
作者:
Wildanger, Dominik;Patton, Brian R.;Schill, Heiko;Marseglia, Luca;Hadden, J. P.;Knauer, Sebastian;Schoenle, Andreas;Rarity, John G.;O'Brien, Jeremy L.;Hell, Stefan W.;Smith, Jason M.

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标准的远场光学显微镜技术提供了对透明样品内部的非侵入性访问,尽管分辨率被限制在光波长λ的一半左右。[1]通过提供不再受衍射限制的分辨率,新兴的远场光学纳米技术正在改变生命科学,但也对材料和信息科学产生了影响。后者的例子是量子计算的概念,依赖于形成耦合量子系统的紧密间隔的晶格中的点缺陷。这种系统的候选者是金刚石中的带负电荷的氮空位(NV)点缺陷,其由位于取代氮旁边的晶格空位组成。NV中心显示出显着的性能作为自旋寄存器,结合在室温下的长相干时间与方便的手段,光学和微波初始化,然后基于荧光的读出。最近的工作表明,相距小于10 nm的NV中心的自旋状态可以在亚微秒的时间尺度上相互通信,这足够快,可以将纠缠量子系统阵列设想为量子处理器的关键一步。[2,3]另一个应用是使用NV中心作为光学传感器。由于它们的光学可寻址自旋状态,这些原子状荧光缺陷可用于磁场和电场计量和生物传感。[4-7]显然,它们的使用将极大地受益于,甚至完全依赖于,在密集的集群或阵列中记录单个中心的可能性。实现纳米级分辨率的第一种方法依赖于在扫描尖端具有NV中心的AFM样配置。[8]但是,像所有近场扫描技术,这些方法是缓慢的,并限于表面。幸运的是,大块金刚石中的NV中心是光稳定的,因此非常适合于具有衍射无限分辨率的远场光学成像。它已被证明,受激发射耗尽(STED)显微镜,可以图像的空间分辨率是10-20倍优于衍射极限的单NV中心。[9,10]虽然相关技术,如基态耗尽显微镜也接近这一水平,STED由于其提供图像作为原始数据的能力,其出色的信噪比,其记录速度以及对样品制备的低要求而保持了其关键作用。[11-13]在这里,我们超越了金刚石中NV中心STED显微镜的先前限制,证明它在原始数据图像中提供了低至2.4±0.3 nm的分辨率。这种记录远场光学分辨率是通过将STED光束聚焦通过制造到金刚石中的固体浸没透镜(SIL)来实现的。[14-16]我们的数据表明,STED和SIL的组合应该非常有效地表征耦合NV自旋的阵列,并推进NV中心的一般应用,特别是它们作为纳米级磁场传感器的用途。STED显微镜通过迫使它们顺序地发出荧光来分离比衍射屏障更近的特征。因此,除了采用光来激发发射体到它们的荧光状态之外,这种纳米方法还使用第二光束,称为STED光束,其强度如此之大,以通过受激辐射去激发来保持发射体不发荧光。同时,STED光束以零点为特征,使得位于零点处或距零点的小距离d/2< λ/4内的特征仍然能够发荧光。因此,标记物可以同时发荧光的空间距离减小到值d<< λ/2,距离.
Standard far-field optical microscopy techniques provide noninvasive access to the interior of transparent samples, albeit with a resolution that is constrained to about half of the wavelength of light λ.[1] By providing a resolution that is no longer limited by diffraction, emerging far-field optical nanoscopy or superresolution techniques are transforming the life sciences, but have also implications in the material and information sciences. Exemplifying the latter are concepts for quantum computation relying on point defects in a closely spaced crystal lattice forming coupled quantum systems. A candidate for such a system is the negatively charged nitrogen vacancy (NV) point defect in diamond, which consists of a lattice vacancy located next to a substitutional nitrogen. The NV center displays remarkable properties as a spin register, combining long coherence times at room temperature with convenient means for optical and microwave initialization followed by fluorescencebased read-out. Recent works have shown that the spin states of NV centers separated< 10 nm apart can communicate with each other on sub-microsecond time scales, which is sufficiently fast to envisage an array of entangled quantum systems as a crucial step towards a quantum processor.[2, 3] Another application is the use of NV centers as optical sensors. Owing to their optically addressable spin state, these atom-like fluorescent defects can be used for magnetic and electric field metrology and bio-sensing.[4–7] Clearly, their use will greatly benefit from, or even fully rely on, the possibility to record individual centers in densely packed clusters or arrays. First approaches to achieve nanometer scale resolutions relied on AFM-like configurations featuring a NV-center at the scanning tip.[8] But like all near-field scanning techniques these approaches are slow and limited to surfaces. Fortunately, NV centers in bulk diamond are photostable and thereby exceptionally well suited for far-field optical imaging with diffractionunlimited resolution. It has been demonstrated that stimulated emission depletion (STED) microscopy, can image single NV-centers with a spatial resolution that is 10–20 times better than the diffraction limit.[9, 10] While related techniques, such as ground state depletion microscopy have also approached this level, STED has maintained its pivotal role due to its ability to provide images as raw data, its outstanding signal-to-noise ratio, its recording speed, and its low demands on sample preparation.[11–13]Here, we surpass previous limits for STED microscopy of NV centers in diamond, demonstrating that it provides a resolution down to 2.4±0.3 nm in raw data images. This record farfield optical resolution is attained by focusing the STED beam through a solid immersion lens (SIL) fabricated into the diamond.[14–16] Our data shows that the combination of STED and SIL should be highly effective to characterize arrays of coupled NV spins and to advance applications of NV centers in general, particularly their use as sensors of nanoscale magnetic fields. STED microscopy separates features that are closer than the diffraction barrier by forcing them to fluoresce sequentially. Therefore, besides employing light for exciting emitters to their fluorescent state, this nanoscopy method uses a second beam, called the STED beam, that is so intense to keep emitters nonfluorescent by stimulated radiative de-excitation. At the same time, the STED beam features a zero so that features located at, or within a small distance d/2< λ/4 from the zero are still capable to fluoresce. Thereby the spatial distance within which markers can fluoresce simultaneously, is reduced to values d<< λ/2, a distance …
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发表时间: 2011-09-01
期刊: NATURE PHYSICS
影响因子: 19.6
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通讯作者: Yacoby, A.
DOI: 10.1209/0295-5075/86/14001
发表时间: 2009-04-01
期刊: EPL
影响因子: 1.8
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通讯作者: Hell, S. W.
DOI: 10.1038/nphys1536
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期刊: NATURE PHYSICS
影响因子: 19.6
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通讯作者: Wrachtrup, J.
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发表时间: 2010-10-04
期刊: SMALL
影响因子: 13.3
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通讯作者: Meijer, Jan
DOI: 10.1038/nmeth.1291
发表时间: 2009-01-01
期刊: NATURE METHODS
影响因子: 48
作者:
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