Microscale-Resolution Thermal Mapping Using a Flexible Platform of Patterned Quantum Sensors.

Temperature sensors with micro- and nanoscale spatial resolution have long been explored for their potential to investigate the details of physical systems at an unprecedented scale. In particular, the rapid miniaturization of transistor technology, with its associated steep boost in power density, calls for sensors that accurately monitor heating distributions. Here, we report on a simple and scalable fabrication approach, based on directed self-assembly and transfer-printing techniques, to constructing arrays of nanodiamonds containing temperature-sensitive fluorescent spin defects. The nanoparticles are embedded within a low-thermal-conductivity matrix that allows for repeated use on a wide range of systems with minimal spurious effects. Additionally, we demonstrate access to a wide spectrum of array parameters ranging from sparser single-particle arrays, with the potential for quantum computing applications, to denser devices with 98 ± 0.8% yield and stronger photoluminescence signals, ideal for temperature measurements. With these, we experimentally reconstruct the temperature map of an operating coplanar waveguide to confirm the accuracy of these platforms.

Isolated electron spins in silicon carbide with millisecond coherence times.

The elimination of defects from SiC has facilitated its move to the forefront of the optoelectronics and power-electronics industries. Nonetheless, because certain SiC defects have electronic states with sharp optical and spin transitions, they are increasingly recognized as a platform for quantum information and nanoscale sensing. Here, we show that individual electron spins in high-purity monocrystalline 4H-SiC can be isolated and coherently controlled. Bound to neutral divacancy defects, these states exhibit exceptionally long ensemble Hahn-echo spin coherence times, exceeding 1 ms. Coherent control of single spins in a material amenable to advanced growth and microfabrication techniques is an exciting route towards wafer-scale quantum technologies.

Engineered micro- and nanoscale diamonds as mobile probes for high-resolution sensing in fluid.

The nitrogen-vacancy (NV) center in diamond is an attractive platform for quantum information and sensing applications because of its room temperature operation and optical addressability. A major research effort focuses on improving the quantum coherence of this defect in engineered micro- and nanoscale diamond particles (DPs), which could prove useful for high-resolution sensing in fluidic environments. In this work we fabricate cylindrical diamonds particles with finely tuned and highly reproducible sizes (diameter and height ranging from 100 to 700 and 500 nm to 2 µm, respectively) using high-purity, single-crystal diamond membranes with shallow-doped NV centers. We show that the spin coherence time of the NV centers in these particles exceeds 700 µs, opening the possibility for the creation of ultrahigh sensitivity micro- and nanoscale sensors. Moreover, these particles can be efficiently transferred into a water suspension and delivered to the region to probe. In particular, we introduce a DP suspension inside a microfluidic circuit and control position and orientation of the particles using an optical trapping apparatus. We demonstrate a DC magnetic sensitivity of 9 µT/√Hz in fluid as well as long-term trapping stability (>30 h), which paves the way toward the use of high-sensitivity pulse techniques on contactless probes manipulated within biological settings.

Influence of Electron Donors on the Charge Transfer Dynamics of Carbon Nanodots in Photocatalytic Systems.

Carbon nanodots (CNDs) are nanosized light-harvesters emerging as next-generation photosensitizers in photocatalytic reactions. Despite their ever-increasing potential applications, the intricacies underlying their photoexcited charge carrier dynamics are yet to be elucidated. In this study, nitrogen-doped graphitic CNDs (NgCNDs) are selectively excited in the presence of methyl viologen (MV2+, redox mediator) and different electron donors (EDs), namely ascorbic acid (AA) and ethylenediaminetetraacetic acid (EDTA). The consequent formation of the methyl viologen radical cation (MV•+) is investigated, and the excited charge carrier dynamics of the photocatalytic system are understood on a 0.1 ps-1 ms time range, providing spectroscopic evidence of oxidative or reductive quenching mechanisms experienced by optically excited NgCNDs (NgCNDs*) depending on the ED implemented. In the presence of AA, NgCNDs* undergo oxidative quenching by MV2+ to form MV•+, which is short-lived due to dehydroascorbic acid, a product of photoinduced hole quenching of oxidized NgCNDs. The EDTA-mediated reductive quenching of NgCNDs* is observed to be at least 2 orders of magnitude slower due to screening by EDTA-MV2+ complexes, but the MV•+ population is stable due to the irreversibly oxidized EDTA preventing a back reaction. In general, our methodology provides a distinct solution with which to study charge transfer dynamics in photocatalytic systems on an extended time range spanning 10 orders of magnitude. This approach generates a mechanistic understanding to select and develop suitable EDs to promote photocatalytic reactions.

Ultrafast melting and recovery of collective order in the excitonic insulator Ta2NiSe5.

The layered chalcogenide Ta2NiSe5 has been proposed to host an excitonic condensate in its ground state, a phase that could offer a unique platform to study and manipulate many-body states at room temperature. However, identifying the dominant microscopic contribution to the observed spontaneous symmetry breaking remains challenging, perpetuating the debate over the ground state properties. Here, using broadband ultrafast spectroscopy we investigate the out-of-equilibrium dynamics of Ta2NiSe5 and demonstrate that the transient reflectivity in the near-infrared range is connected to the system's low-energy physics. We track the status of the ordered phase using this optical signature, establishing that high-fluence photoexcitations can suppress this order. From the sub-50 fs quenching timescale and the behaviour of the photoinduced coherent phonon modes, we conclude that electronic correlations provide a decisive contribution to the excitonic order formation. Our results pave the way towards the ultrafast control of an exciton condensate at room temperature.

Imaging the coherent propagation of collective modes in the excitonic insulator Ta2NiSe5 at room temperature.

Excitonic insulators host a condensate of electron-hole pairs at equilibrium, giving rise to collective many-body effects. Although several materials have emerged as excitonic insulator candidates, evidence of long-range coherence is lacking and the origin of the ordered phase in these systems remains controversial. Here, using ultrafast pump-probe microscopy, we investigate the possible excitonic insulator Ta2NiSe5 Below 328 K, we observe the anomalous micrometer-scale propagation of coherent modes at velocities of ~105 m/s, which we attribute to the hybridization between phonon modes and the phase mode of the condensate. We develop a theoretical framework to support this explanation and propose that electronic interactions provide a substantial contribution to the ordered phase in Ta2NiSe5 These results allow us to understand how the condensate's collective modes transport energy and interact with other degrees of freedom. Our study provides a unique paradigm for the investigation and manipulation of these properties in strongly correlated materials.