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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Color-center–hosting semiconductors are emerging as promising source materials for low-field dynamic nuclear polarization (DNP) at or near room temperature, but hyperfine broadening, susceptibility to magnetic field heterogeneity, and nuclear spin relaxation induced by other paramagnetic defects set practical constraints difficult to circumvent. Here, we explore an alternate route to color-center–assisted DNP using nitrogen-vacancy (NV) centers in diamond coupled to substitutional nitrogen impurities, the so-called P1 centers. Working near the level anticrossing condition—where the P1 Zeeman splitting matches one of the NV spin transitions—we demonstrate efficient microwave-free 13 C DNP through the use of consecutive magnetic field sweeps and continuous optical excitation. The amplitude and sign of the polarization can be controlled by adjusting the low-to-high and high-to-low magnetic field sweep rates in each cycle so that one is much faster than the other. By comparing the 13 C DNP response for different crystal orientations, we show that the process is robust to magnetic field/NV misalignment, a feature that makes the present technique suitable to diamond powders and settings where the field is heterogeneous. Applications to shallow NVs could capitalize on the greater physical proximity between surface paramagnetic defects and outer nuclei to efficiently polarize target samples in contact with the diamond crystal.more » « less
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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.
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Abstract The nitrogen-vacancy (NV) color center in diamond has rapidly emerged as an important solid-state system for quantum information processing. Whereas individual spin registers have been used to implement small-scale diamond quantum computing, the realization of a large-scale device requires the development of an on-chip quantum bus for transporting information between distant qubits. Here, we propose a method for coherent quantum transport of an electron and its spin state between distant NV centers. Transport is achieved by the implementation of spatial stimulated adiabatic Raman passage through the optical control of the NV center charge states and the confined conduction states of a diamond nanostructure. Our models show that, for two NV centers in a diamond nanowire, high-fidelity transport can be achieved over distances of order hundreds of nanometers in timescales of order hundreds of nanoseconds. Spatial adiabatic passage is therefore a promising option for realizing an on-chip spin quantum bus.more » « less
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Abstract Herein, the role that point defects have played over the last two decades in realizing solid‐state laser refrigeration is discussed. A brief introduction to the field of solid‐state laser refrigeration is given with an emphasis on the fundamental physical phenomena and quantized electronic transitions that have made solid‐state laser‐cooling possible. Lanthanide‐based point defects, such as trivalent ytterbium ions (Yb3+), have played a central role in the first demonstrations and subsequent development of advanced materials for solid‐state laser refrigeration. Significant discussion is devoted to the quantum mechanical description of optical transitions in lanthanide ions, and their influence on laser cooling. Transition‐metal point defects have been shown to generate substantial background absorption in ceramic materials, decreasing the overall efficiency of a particular laser refrigeration material. Other potential color centers based on fluoride vacancies with multiple potential charge states are also considered. In conclusion, novel materials for solid‐state laser refrigeration, including color centers in diamond that have recently been proposed to realize the solid‐state laser refrigeration of semiconducting materials, are discussed.
- Free Publicly Accessible Full Text
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Accepted Manuscript1.0
- Journal Article:
- https://doi.org/10.1126/sciadv.abl9402
