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Magnetic resonance spectroscopy of single biomolecules under near-physiological conditions may substantially advance understanding of biological function, yet remains very challenging. Here we use nitrogen-vacancy centers in diamonds to detect electron spin resonance spectra of individual, tethered DNA duplexes labeled with a nitroxide spin label in aqueous buffer solutions at ambient temperatures. This paves the way for magnetic resonance studies on single biomolecules and their inter-molecular interactions in a native-like environment.
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We report on a detailed characterization of complex dielectric response of Na-DNA aqueous solutions by means of low-frequency dielectric spectroscopy (40 Hz - 110 MHz). Results reveal two broad relaxation modes of strength 20<Deltaepsilon_LF<100 and 5<Deltaepsilon_HF<20, centered at 0.5 kHz< u_LF<70 kHz and 0.1 MHz< u_HF<15 MHz. The characteristic length scale of the LF process, 50<L_LF<750nm, scales with DNA concentration as c_DNA^{-0.29pm0.04} and is independent of the ionic strength in the low added salt regime. Conversely, the measured length scale of the LF process does not vary with DNA concentration but depends on the ionic strength of the added salt as I_s^{-1} in the high added salt regime. On the other hand, the characteristic length scale of the HF process, 3<L_HF<50 nm, varyes with DNA concentration as c_DNA^{-0.5} for intermediate and large DNA concentrations. At low DNA concentrations and in the low added salt limit the characteristic length scale of the HF process scales as c_DNA^{-0.33}. We put these results in perspective regarding the integrity of the double stranded form of DNA at low salt conditions as well as regarding the role of different types of counterions in different regimes of dielectric dispersion. We argue that the free DNA counterions are primarily active in the HF relaxation, while the condensed counterions play a role only in the LF relaxation. We also suggest theoretical interpretations for all these length scales in the whole regime of DNA and salt concentrations and discuss their ramifications and limitations.
We report on sensing stability of nanodiamond (ND) quantum sensors in various pH aqueous buffer solutions for the two detection schemes of quantum decoherence spectroscopy and thermometry. The electron spin properties of single nitrogen-vacancy (NV) centers in 25-nm-sized NDs have been characterized by a spin-measurement compatible perfusion (SMCP) chamber where observing the same individual NDs in different buffer solutions is possible. With this system, we have determined the stability of the NV quantum sensors during the pH change from 4 to 11 as the fluctuations of +- 12% and +- 0.2 MHz for the spin coherence time ($T_2$) and the resonance frequency ($omega_0$) of their mean values, which are comparable to the instrumental error of the measurement system. Here, we discuss the importance of characterizing the sensing stability during pH changes and how the present observations affect ND-based NV quantum sensing.
Electron spin resonance (ESR) spectroscopy has broad applications in physics, chemistry and biology. As a complementary tool, zero-field ESR (ZF-ESR) spectroscopy has been proposed for decades and shown its own benefits for investigating the electron fine and hyperfine interaction. However, the ZF-ESR method has been rarely used due to the low sensitivity and the requirement of much larger samples than conventional ESR. In this work, we present a method for deploying ZF-ESR spectroscopy at the nanoscale by using a highly sensitive quantum sensor, the nitrogen-vacancy center in diamond. We also measure the nanoscale ZF-ESR spectrum of a few P1 centers in diamond, and show that the hyperfine coupling constant can be directly extracted from the spectrum. This method opens the door to practical applications of ZF-ESR spectroscopy, such as investigation of the structure and polarity information in spin-modified organic and biological systems.
We report electron spin resonance measurements of donors in silicon at millikelvin temperatures using a superconducting $LC$ planar micro-resonator and a Josephson Parametric Amplifier. The resonator includes a nanowire inductor, defining a femtoliter detection volume. Due to strain in the substrate, the donor resonance lines are heavily broadened. Single-spin to photon coupling strengths up to $sim 3~text{kHz}$ are observed. The single shot sensitivity is $120 pm 24~$spins/Hahn echo, corresponding to $approx 12 pm 3$~spins$/sqrt{text{Hz}}$ for repeated acquisition.
Electron paramagnetic resonance (EPR) spectroscopy is an important technology in physics, chemistry, materials science, and biology. Sensitive detection with a small sample volume is a key objective in these areas, because it is crucial, for example, for the readout of a highly packed spin based quantum memory or the detection of unlabeled metalloproteins in a single cell. In conventional EPR spectrometers, the energy transfer from the spins to the cavity at a Purcell enhanced rate plays an essential role and requires the spins to be resonant with the cavity, however the size of the cavity (limited by the wavelength) makes it difficult to improve the spatial resolution. Here, we demonstrate a novel EPR spectrometer using a single artificial atom as a sensitive detector of spin magnetization. The artificial atom, a superconducting flux qubit, provides advantages both in terms of its quantum properties and its much stronger coupling with magnetic fields. We have achieved a sensitivity of $sim$400 spins/$sqrt{mathrm{Hz}}$ with a magnetic sensing volume around $10^{-14} lambda^3$ (50 femto-liters). This corresponds to an improvement of two-order of magnitude in the magnetic sensing volume compared with the best cavity based spectrometers while maintaining a similar sensitivity as those spectrometers . Our artificial atom is suitable for scaling down and thus paves the way for measuring single spins on the nanometer scale.
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