The detection of ensembles of spins under ambient conditions has revolutionized the biological, chemical, and physical sciences through magnetic resonance imaging and nuclear magnetic resonance. Pushing sensing capabilities to the individual-spin lev
el would enable unprecedented applications such as single molecule structural imaging; however, the weak magnetic fields from single spins are undetectable by conventional far-field resonance techniques. In recent years, there has been a considerable effort to develop nanoscale scanning magnetometers, which are able to measure fewer spins by bringing the sensor in close proximity to its target. The most sensitive of these magnetometers generally require low temperatures for operation, but measuring under ambient conditions (standard temperature and pressure) is critical for many imaging applications, particularly in biological systems. Here we demonstrate detection and nanoscale imaging of the magnetic field from a single electron spin under ambient conditions using a scanning nitrogen-vacancy (NV) magnetometer. Real-space, quantitative magnetic-field images are obtained by deterministically scanning our NV magnetometer 50 nanometers above a target electron spin, while measuring the local magnetic field using dynamically decoupled magnetometry protocols. This single-spin detection capability could enable single-spin magnetic resonance imaging of electron spins on the nano- and atomic scales and opens the door for unique applications such as mechanical quantum state transfer.
Quantum control of individual spins in condensed matter systems is an emerging field with wide-ranging applications in spintronics, quantum computation, and sensitive magnetometry. Recent experiments have demonstrated the ability to address and manip
ulate single electron spins through either optical or electrical techniques. However, it is a challenge to extend individual spin control to nanoscale multi-electron systems, as individual spins are often irresolvable with existing methods. Here we demonstrate that coherent individual spin control can be achieved with few-nm resolution for proximal electron spins by performing single-spin magnetic resonance imaging (MRI), which is realized via a scanning magnetic field gradient that is both strong enough to achieve nanometric spatial resolution and sufficiently stable for coherent spin manipulations. We apply this scanning field-gradient MRI technique to electronic spins in nitrogen-vacancy (NV) centers in diamond and achieve nanometric resolution in imaging, characterization, and manipulation of individual spins. For NV centers, our results in individual spin control demonstrate an improvement of nearly two orders of magnitude in spatial resolution compared to conventional optical diffraction-limited techniques. This scanning-field-gradient microscope enables a wide range of applications including materials characterization, spin entanglement, and nanoscale magnetometry.
Hanle effect is ubiquitous in the study of spin-related phenomena and has been used to determine spin lifetime, precession and transport in semiconductors. Here, we report an experimental observation of anomalous Hanle effect in individual self-assem
bled InAs/GaAs quantum dots where we find that a sizeable photo-created electron spin polarization can be maintained in transverse fields as high as 1T until it abruptly collapses. The striking broadening of the Hanle curve by a factor of ~20 and its bistability upon reversal of the magnetic sweep direction points to a novel dynamical nuclear spin polarization mechanism where the effective nuclear magnetic field compensates the transverse applied field. This interpretation is further supported by the measurement of actual electron Zeeman splitting which exhibits an abrupt increase at the Hanle curve collapse. Strong inhomogeneous quadrupolar interactions typical for strained quantum dots are likely to play a key role in polarizing nuclear spins perpendicular to the optically injected spin orientation.
The physics of interacting nuclear spins arranged in a crystalline lattice is typically described using a thermodynamic framework: a variety of experimental studies in bulk solid-state systems have proven the concept of a spin temperature to be not o
nly correct but also vital for the understanding of experimental observations. Using demagnetization experiments we demonstrate that the mesoscopic nuclear spin ensemble of a quantum dot (QD) can in general not be described by a spin temperature. We associate the observed deviations from a thermal spin state with the presence of strong quadrupolar interactions within the QD that cause significant anharmonicity in the spectrum of the nuclear spins. Strain-induced, inhomogeneous quadrupolar shifts also lead to a complete suppression of angular momentum exchange between the nuclear spin ensemble and its environment, resulting in nuclear spin relaxation times exceeding an hour. Remarkably, the position dependent axes of quadrupolar interactions render magnetic field sweeps inherently non-adiabatic, thereby causing an irreversible loss of nuclear spin polarization.
