Solid-state laser refrigeration of semiconductors remains an outstanding experimental challenge. In this work, we show that, following excitation with a laser wavelength of 532 nm, bulk diamond crystals doped with H3 centers both emit efficient up-conversion (anti-Stokes) photoluminescence and also show significantly reduced photothermal heating relative to crystals doped with nitrogen–vacancy (NV) centers. The H3 center in diamond is a highly photostable defect that avoids bleaching at high laser irradiances of 10–70 MW/cm[Formula: see text] and has been shown to exhibit laser action, tunable over the visible band of 500–600 nm. The observed reduction of photothermal heating arises due to a decrease in the concentration of absorbing point defects, including NV-centers. These results encourage future exploration of techniques for H3 enrichment in diamonds under high-pressure, high-temperature conditions for the simultaneous anti-Stokes fluorescence cooling and radiation balanced lasing in semiconductor materials. Reducing photothermal heating in diamond through the formation of H3 centers also opens up new possibilities in quantum sensing via optically detected magnetic resonance spectroscopy at ambient conditions.
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Imaging dark charge emitters in diamond via carrier-to-photon conversion
The application of color centers in wide-bandgap semiconductors to nanoscale sensing and quantum information processing largely rests on our knowledge of the surrounding crystalline lattice, often obscured by the countless classes of point defects the material can host. Here, we monitor the fluorescence from a negatively charged nitrogen-vacancy (NV − ) center in diamond as we illuminate its vicinity. Cyclic charge state conversion of neighboring point defects sensitive to the excitation beam leads to a position-dependent stream of photo-generated carriers whose capture by the probe NV − leads to a fluorescence change. This “charge-to-photon” conversion scheme allows us to image other individual point defects surrounding the probe NV, including nonfluorescent “single-charge emitters” that would otherwise remain unnoticed. Given the ubiquity of color center photochromism, this strategy may likely find extensions to material systems other than diamond.
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- NSF-PAR ID:
- 10338229
- Date Published:
- Journal Name:
- Science Advances
- Volume:
- 8
- Issue:
- 1
- ISSN:
- 2375-2548
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract Nitrogen-vacancy (NV) and silicon-vacancy (SiV) color defects in diamond are promising systems for applications in quantum technology. The NV and SiV centers have multiple charge states, and their charge states have different electronic, optical and spin properties. For the NV centers, most investigations for quantum sensing applications are targeted on the negatively charged NV (NV−), and it is important for the NV centers to be in the NV−state. However, it is known that the NV centers are converted to the neutrally charged state (NV0) under laser excitation. An energetically favorable charge state for the NV and SiV centers depends on their local environments. It is essential to understand and control the charge state dynamics for their quantum applications. In this work, we discuss the charge state dynamics of NV and SiV centers under high-voltage nanosecond pulse discharges. The NV and SiV centers coexist in the diamond crystal. The high-voltage pulses enable manipulating the charge states efficiently. These voltage-induced changes in charge states are probed by their photoluminescence spectral analysis. The analysis result from the present experiment shows that the high-voltage nanosecond pulses cause shifts of the chemical potential and can convert the charge states of NV and SiV centers with the transition rates of ∼MHz. This result also indicates that the major population of the SiV centers in the sample is the doubly negatively charged state (SiV2−), which is often overlooked because of its non-fluorescent and non-magnetic nature. This demonstration paves a path for a method of rapid manipulation of the NV and SiV charge states in the future.
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1126/sciadv.abl9402
