基于金刚石室温固态单自旋体系的微观磁共振实验研究
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摘要
自旋磁共振是物质科学领域的一个基本物理现象,它描述处于外磁场中的原子核或者电子自旋,能够吸收和放出对应频率的电磁辐射,即发生磁共振现象。自旋在物质中广泛存在,因而自旋磁共振技术能够用来准确、快速和无破坏性地获取物质的组成和结构上的信息,是当代科学中最为重要的物质探索技术之一。当前的自旋磁共振谱仪基于系综探测原理,它的测试对象是含有百亿个以上相同自旋的系综样品。然而,近年来随着物质科学探索的不断深入,人们开始逐渐从统计平均测量向直接探测单量子的信息迈进。在自旋磁共振领域,实现微观磁共振,甚至单自旋磁共振是这一方向发展的极为重要的科学目标。为实现这一科学目标,我们选取了基于掺杂金刚石中氮-空位(NV)对的固态单自旋作为探针,此体系室温下退相干时间长达毫秒量级、可用光学共聚焦系统实现初始化和检测,在室温下实现单电子自旋量子态调控和检测。代替传统的电探测方式,用基于此体系单自旋态制备成量子干涉仪,将微观自旋体系产生的弱磁信号转为干涉仪的相位,从而实现高灵敏度的信号检测,这也是用此体系实现微观磁共振、甚至单自旋磁共振的必要条件。最终的目标是实现单分子探测与成像,这在物理、化学、生物、材料等领域都具有广泛而重要的应用前景。
我们围绕这一核心目标开展了相关的实验研究,本论文主要内容是介绍我们在自搭建的光探测磁共振实验平台上,完成的室温单自旋量子调控及高分辨率精密信号探测的相关成果。主体分成如下三个阶段的工作：
1.我们建设了一套多波段光探测磁共振平台并在其上实现了室温单自旋量子调控,实验上实现了此体系上的第一个量子算法。接着,又应用动力学去耦技术到单自旋体系,观测到反常退相干效应,研究了NV探针的退相干机制,实现了精密的相位测量。而连续波去耦与逻辑门操作结合,使我们可以实现长时间高保真度的量子调控。
2.基于以上量子调控技术,我们首先实验实现了单电子暗自旋的探测及调控,我们不仅在实验上探测到了16纳米远处的单暗电子自旋并得到其连续波谱,还将其初始化、调控和读出,发掘其作为量子寄存器的潜力。接着不同于以往对体内单核自旋的探测,我们成功探测到自旋簇,并通过计算得到其耦合强度及空间结构,这是实现大分子结构的探测可行途径之一,另外,对研究多体相互作用及演化提供了新的手段。
3.核磁共振谱是目前应用范围最广的谱学技术,已经广泛应用于科研及医学等领域。但是,在室温下实现纳米尺度的核磁共振是一个巨大的挑战。我们通过多次尝试及技术的改进,最终利用掺杂金刚石中距表面～7纳米深度的氮-空位单电子自旋作为原子尺度磁探针,分别实现了(5nm)3体积液钵和固体有机样品中质子信号的检测,其中包括的质子总数约为二万个,其产生的磁信号强度相当于100个统计极化的核自旋。
As one of the most important exploring technologies in modern science, the spin magnetic resonance technology is capable of obtaining information of sub-jects composition and structure in an accurate, rapid and non-destructive way. At present nuclear magnetic resonance spectroscopy is the most popular spectroscopy, widely used in scientific research and medical fields. Current spin-magnetic reso-nance spectrometers are based on the principle of ensemble detection and the test object is an ensemble sample containing billions of identical spins. However, at room temperature NMR at nano-scale is still a huge challenge.
To achieve the scientific goal, we choose single spins in solids based on NV defect center in diamond-(NV) as the sensitivity magnetic probe. The single NV spin can be easily visualized, polarized and detected with a confocal microscope. Ultra-long spin coherence time for such qubits, even at room temperature, enables it is ultra-sensitivity to external magnetic noise with characteristic frequency. Instead of traditional electrical defect, weak magnetic signals generated by the nano-scale spin system is mapped to coherent state phase, so as to realize high sensitivity signal detection.
1. We designed and constructed the S-band Optical Detected Magnetic Reso-nance spectrometers to meet the requirement of the quantum manipulation on single NV spin at room temperature. We implemented the first quantum algorithm on the single spin system. Then, we succeed to transfer the widely used dynamical decoupling technology to our NV system. Then we observed the anomalous decoherence effect in a quantum bath at room temperature, enhanced phase estimation in a multi-pass quantum metrology protocol, and protected quantum gate by continuous dynamical decoupling.
2. Based on the above technology, we sensed a dark electron spin located16nm from NV center and manipulated it by Double Electron-Electron Resonance methods. Besides, instead of single nuclear spin, we sensed a single13C-13C nuclear spin dimer located1nm from the NV center and characterized the interaction between the two nuclear spins. These results demonstrate that central spin decoherence under dynamical decoupling control is a feasible probe for NMR structure analysis of single molecules.
3. Application of nuclear magnetic resonance (NMR) spectroscopy to nanoscale samples has remained an elusive goal, achieved only with great experimental effort at subkelvin temperatures. We demonstrated detection of NMR sig-nals from a (5-nanometer)3voxel of various fluid and solid organic samples under ambient conditions. We used an atomic-size magnetic field sensor, a single nitrogen-vacancy defect center, embedded～7nanometers under the surface of a bulk diamond to record NMR spectra of various samples placed on the diamond surface. Its detection volume consisted of only104nuclear spins with a net magnetization of only102statistically polarized spins.
我们围绕这一核心目标开展了相关的实验研究,本论文主要内容是介绍我们在自搭建的光探测磁共振实验平台上,完成的室温单自旋量子调控及高分辨率精密信号探测的相关成果。主体分成如下三个阶段的工作：
1.我们建设了一套多波段光探测磁共振平台并在其上实现了室温单自旋量子调控,实验上实现了此体系上的第一个量子算法。接着,又应用动力学去耦技术到单自旋体系,观测到反常退相干效应,研究了NV探针的退相干机制,实现了精密的相位测量。而连续波去耦与逻辑门操作结合,使我们可以实现长时间高保真度的量子调控。
2.基于以上量子调控技术,我们首先实验实现了单电子暗自旋的探测及调控,我们不仅在实验上探测到了16纳米远处的单暗电子自旋并得到其连续波谱,还将其初始化、调控和读出,发掘其作为量子寄存器的潜力。接着不同于以往对体内单核自旋的探测,我们成功探测到自旋簇,并通过计算得到其耦合强度及空间结构,这是实现大分子结构的探测可行途径之一,另外,对研究多体相互作用及演化提供了新的手段。
3.核磁共振谱是目前应用范围最广的谱学技术,已经广泛应用于科研及医学等领域。但是,在室温下实现纳米尺度的核磁共振是一个巨大的挑战。我们通过多次尝试及技术的改进,最终利用掺杂金刚石中距表面～7纳米深度的氮-空位单电子自旋作为原子尺度磁探针,分别实现了(5nm)3体积液钵和固体有机样品中质子信号的检测,其中包括的质子总数约为二万个,其产生的磁信号强度相当于100个统计极化的核自旋。
As one of the most important exploring technologies in modern science, the spin magnetic resonance technology is capable of obtaining information of sub-jects composition and structure in an accurate, rapid and non-destructive way. At present nuclear magnetic resonance spectroscopy is the most popular spectroscopy, widely used in scientific research and medical fields. Current spin-magnetic reso-nance spectrometers are based on the principle of ensemble detection and the test object is an ensemble sample containing billions of identical spins. However, at room temperature NMR at nano-scale is still a huge challenge.
To achieve the scientific goal, we choose single spins in solids based on NV defect center in diamond-(NV) as the sensitivity magnetic probe. The single NV spin can be easily visualized, polarized and detected with a confocal microscope. Ultra-long spin coherence time for such qubits, even at room temperature, enables it is ultra-sensitivity to external magnetic noise with characteristic frequency. Instead of traditional electrical defect, weak magnetic signals generated by the nano-scale spin system is mapped to coherent state phase, so as to realize high sensitivity signal detection.
1. We designed and constructed the S-band Optical Detected Magnetic Reso-nance spectrometers to meet the requirement of the quantum manipulation on single NV spin at room temperature. We implemented the first quantum algorithm on the single spin system. Then, we succeed to transfer the widely used dynamical decoupling technology to our NV system. Then we observed the anomalous decoherence effect in a quantum bath at room temperature, enhanced phase estimation in a multi-pass quantum metrology protocol, and protected quantum gate by continuous dynamical decoupling.
2. Based on the above technology, we sensed a dark electron spin located16nm from NV center and manipulated it by Double Electron-Electron Resonance methods. Besides, instead of single nuclear spin, we sensed a single13C-13C nuclear spin dimer located1nm from the NV center and characterized the interaction between the two nuclear spins. These results demonstrate that central spin decoherence under dynamical decoupling control is a feasible probe for NMR structure analysis of single molecules.
3. Application of nuclear magnetic resonance (NMR) spectroscopy to nanoscale samples has remained an elusive goal, achieved only with great experimental effort at subkelvin temperatures. We demonstrated detection of NMR sig-nals from a (5-nanometer)3voxel of various fluid and solid organic samples under ambient conditions. We used an atomic-size magnetic field sensor, a single nitrogen-vacancy defect center, embedded～7nanometers under the surface of a bulk diamond to record NMR spectra of various samples placed on the diamond surface. Its detection volume consisted of only104nuclear spins with a net magnetization of only102statistically polarized spins.
引文
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