Initiating and Monitoring the Evolution of Single Electrons Within Atom-Defined Structures.

Using a noncontact atomic force microscope, we track and manipulate the position of single electrons confined to atomic structures engineered from silicon dangling bonds on the hydrogen terminated silicon surface. An attractive tip surface interaction mechanically manipulates the equilibrium position of a surface silicon atom, causing rehybridization that stabilizes a negative charge at the dangling bond. This is applied to controllably switch the charge state of individual dangling bonds. Because this mechanism is based on short range interactions and can be performed without applied bias voltage, we maintain both site-specific selectivity and single-electron control. We extract the short range forces involved with this mechanism by subtracting the long range forces acquired on a dimer vacancy site. As a result of relaxation of the silicon lattice to accommodate negatively charged dangling bonds, we observe charge configurations of dangling bond structures that remain stable for many seconds at 4.5 K. Subsequently, we use charge manipulation to directly prepare the ground state and metastable charge configurations of dangling bond structures composed of up to six atoms.

Strong microwave squeezing above 1 Tesla and 1 Kelvin.

Squeezed states of light have been used extensively to increase the precision of measurements, from the detection of gravitational waves to the search for dark matter. In the optical domain, high levels of vacuum noise squeezing are possible due to the availability of low loss optical components and high-performance squeezers. At microwave frequencies, however, limitations of the squeezing devices and the high insertion loss of microwave components make squeezing vacuum noise an exceptionally difficult task. Here we demonstrate direct measurements of high levels of microwave squeezing. We use an ultra-low loss setup and weakly-nonlinear kinetic inductance parametric amplifiers to squeeze microwave noise 7.8(2) dB below the vacuum level. The amplifiers exhibit a resilience to magnetic fields and permit the demonstration of large squeezing levels inside fields of up to 2 T. Finally, we exploit the high critical temperature of our amplifiers to squeeze a warm thermal environment, achieving vacuum level noise at a temperature of 1.8 K. These results enable experiments that combine squeezing with magnetic fields and permit quantum-limited microwave measurements at elevated temperatures, significantly reducing the complexity and cost of the cryogenic systems required for such experiments.

Latched detection of zeptojoule spin echoes with a kinetic inductance parametric oscillator.

When strongly pumped at twice their resonant frequency, nonlinear resonators develop a high-amplitude intracavity field, a phenomenon known as parametric self-oscillations. The boundary over which this instability occurs can be extremely sharp and thereby presents an opportunity for realizing a detector. Here, we operate such a device based on a superconducting microwave resonator whose nonlinearity is engineered from kinetic inductance. The device indicates the absorption of low-power microwave wavepackets by transitioning to a self-oscillating state. Using calibrated pulses, we measure the detection efficiency to zeptojoule energy wavepackets. We then apply it to measurements of electron spin resonance, using an ensemble of 209Bi donors in silicon that are inductively coupled to the resonator. We achieve a latched readout of the spin signal with an amplitude that is five hundred times greater than the underlying spin echoes.

In situ amplification of spin echoes within a kinetic inductance parametric amplifier.

The use of superconducting microresonators together with quantum-limited Josephson parametric amplifiers has enhanced the sensitivity of pulsed electron spin resonance (ESR) measurements by more than four orders of magnitude. So far, the microwave resonators and amplifiers have been designed as separate components due to the incompatibility of Josephson junction-based devices with magnetic fields. This has produced complex spectrometers and raised technical barriers toward adoption of the technique. Here, we circumvent this issue by coupling an ensemble of spins directly to a weakly nonlinear and magnetic field-resilient superconducting microwave resonator. We perform pulsed ESR measurements with a 1-pL mode volume containing 6 × 107 spins and amplify the resulting signals within the device. When considering only those spins that contribute to the detected signals, we find a sensitivity of [Formula: see text] for a Hahn echo sequence at a temperature of 400 mK. In situ amplification is demonstrated at fields up to 254 mT, highlighting the technique's potential for application under conventional ESR operating conditions.

All-electronic Nanosecond-resolved Scanning Tunneling Microscopy: Facilitating the Investigation of Single Dopant Charge Dynamics.

The miniaturization of semiconductor devices to scales where small numbers of dopants can control device properties requires the development of new techniques capable of characterizing their dynamics. Investigating single dopants requires sub-nanometer spatial resolution, which motivates the use of scanning tunneling microscopy (STM). However, conventional STM is limited to millisecond temporal resolution. Several methods have been developed to overcome this shortcoming, including all-electronic time-resolved STM, which is used in this study to examine dopant dynamics in silicon with nanosecond resolution. The methods presented here are widely accessible and allow for local measurement of a wide variety of dynamics at the atomic scale. A novel time-resolved scanning tunneling spectroscopy technique is presented and used to efficiently search for dynamics.

Visible-Light Actinometry and Intermittent Illumination as Convenient Tools to Study Ru(bpy)3Cl2 Mediated Photoredox Transformations.

Photoredox catalysis provides many green opportunities for radical-mediated synthetic transformations. However, the determination of the underlying mechanisms has been challenging due to lack of quantitative methods that can be easily implemented in synthetic labs, where this research tends to be centered. We report here on the development, characterization and calibration of a novel actinometer based on the photocatalyst tris(2,2'-bipyridyl)ruthenium(II) chloride (Ru(bpy)3Cl2). By using the same molecule as the photocatalyst and the actinometer, we eliminate problems associated with matching sample spectral distribution, lamp-sample spectral overlap and other problems intrinsic to doing quantitative photochemistry in a laboratory that has little expertise in this area. In order to validate our actinometer system in determining the quantum yield of a Ru(bpy)3Cl2 photosensitized reaction, we test the Ru(bpy)3Cl2 catalyzed oxidation of benzhydrol to benzophenone as a model chain reaction. We also revive the rotating sector method by updating the technique for modern LED technologies and demonstrate how intermittent illumination on the timescale of milliseconds to seconds can help probe a chain reaction, using the benzhydrol to benzophenone oxidation to validate the technique. We envision these methods to have great implications in the field of photoredox catalysis, providing researchers with valuable research tools.