skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: Optical Properties of Low‐Defect Large‐Area Hexagonal Boron Nitride for Quantum Applications
Intrinsic defects and their concentrations in hexagonal boron nitride (h‐BN) play a key role in single‐photon emission. In this study, the optical properties of large‐area multilayer h‐BN‐on‐sapphire grown by metal‐organic chemical vapor deposition are explored. Based on the detailed spectroscopic characterization using both cathodoluminescence (CL) and photoluminescence (PL) measurements, the material is devoid of random single‐point defects instead of a few clustered complex defects. The emission spectra of the measurements confirm a record‐low‐defect concentration of ≈104 cm−2. Post‐annealing, no significant changes are observed in the measured spectra and the defect concentrations remain unaltered. Through CL and PL spectroscopy, an optically active boron vacancy spin defect is identified and a novel complex defect combination arising from carbon impurities is revealed. This complex defect, previously unreported, signifies a unique aspect of the material. In these findings, the understanding of defect‐induced optical properties in h‐BN films is contributed, providing insights for potential applications in quantum information science.  more » « less
Award ID(s):
2011876
PAR ID:
10514817
Author(s) / Creator(s):
 ;  ;  ;  ;  ;  ;  ;  
Publisher / Repository:
Wiley Blackwell (John Wiley & Sons)
Date Published:
Journal Name:
physica status solidi (RRL) – Rapid Research Letters
Volume:
18
Issue:
6
ISSN:
1862-6254
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. A series of atomic-like photoluminescence (PL) emission peaks in UV region near 4.0 eV were created by thermal annealing hexagonal boron nitride (h-BN) single crystals in air. The pristine h-BN did not have these peaks, emitting strong phonon-assisted band edge PL with peaks at 5.78 and 5.89 eV. After annealing the h-BN crystals in ambient air, a new atomic-like sharp emission in UV region at 4.09 eV with a line width of 0.2 nm appeared along with its phonon replicas at 3.89 and 3.69 eV in the low temperature (8 K) PL measurement. Further testing demonstrated that annealing the h-BN samples in the temperature window of 700–950 °C for 60 min generated the atomic-like emission. The peak position of the emission line is stable with the temperature and PL excitation power. Our study also suggests that the defect responsible for the atomic-like emission resides in the surface region. 
    more » « less
  2. Color centers in wide bandgap semiconductors are attracting broad attention for use as platforms for quantum technologies relying on room-temperature single-photon emission (SPE), and for nanoscale metrology applications building on the centers’ response to electric and magnetic fields. Here, we demonstrate room-temperature SPE from defects in cubic boron nitride (cBN) nanocrystals, which we unambiguously assign to the cubic phase using spectrally resolved Raman imaging. These isolated spots show photoluminescence (PL) spectra with zero-phonon lines (ZPLs) within the visible region (496–700 nm) when subject to sub-bandgap laser excitation. Second-order autocorrelation of the emitted photons reveals antibunching withg2(0) ∼ 0.2, and a decay constant of 2.75 ns that is further confirmed through fluorescence lifetime measurements. The results presented herein prove the existence of optically addressable isolated quantum emitters originating from defects in cBN, making this material an interesting platform for opto-electronic devices and quantum applications. 
    more » « less
  3. Abstract The recent observation of unusually high thermal conductivity exceeding 1000 W m−1K−1in single‐crystal boron arsenide (BAs) has led to interest in the potential application of this semiconductor for thermal management. Although both the electron/hole high mobilities have been calculated for BAs, there is a lack of experimental investigation of its electronic properties. Here, a photoluminescence (PL) measurement of single‐crystal BAs at different temperatures and pressures is reported. The measurements reveal an indirect bandgap and two donor–acceptor pair (DAP) recombination transitions. Based on first‐principles calculations and time‐of‐flight secondary‐ion mass spectrometry results, the two DAP transitions are confirmed to originate from Si and C impurities occupying shallow energy levels in the bandgap. High‐pressure PL spectra show that the donor level with respect to the conduction band minimum shrinks with increasing pressure, which affects the release of free carriers from defect states. These findings suggest the possibility of strain engineering of the transport properties of BAs for application in electronic devices. 
    more » « less
  4. Abstract The development of tandem photovoltaics and photoelectrochemical solar cells requires new absorber materials with bandgaps in the range of ≈1.5–2.3 eV, for use in the top cell paired with a narrower‐gap bottom cell. An outstanding challenge is finding materials with suitable optoelectronic and defect properties, good operational stability, and synthesis conditions that preserve underlying device layers. This study demonstrates the Zintl phosphide compound CaZn2P2as a compelling candidate semiconductor for these applications. Phase‐pure, ≈500 nm‐thick CaZn2P2thin films are prepared using a scalable reactive sputter deposition process at growth temperatures as low as 100 °C, which is desirable for device integration. Ultraviolet‐visible  spectroscopy shows that CaZn2P2films exhibit an optical absorptivity of ≈104 cm−1at ≈1.95 eV direct bandgap. Room‐temperature photoluminescence (PL) measurements show near‐band‐edge optical emission, and time‐resolved microwave conductivity (TRMC) measurements indicate a photoexcited carrier lifetime of ≈30 ns. CaZn2P2is highly stable in both ambient conditions and moisture, as evidenced by PL and TRMC measurements. Experimental data are supported by first‐principles calculations, which indicate the absence of low‐formation‐energy, deep intrinsic defects. Overall, this study shall motivate future work integrating this potential top cell absorber material into tandem solar cells. 
    more » « less
  5. Color centers in hexagonal boron nitride (hBN) are presently attracting broad interest as a novel platform for nanoscale sensing and quantum information processing. Unfortunately, their atomic structures remain largely elusive and only a small percentage of the emitters studied thus far have the properties required to serve as optically addressable spin qubits. Here, we use confocal fluorescence microscopy at variable temperatures to study a new class of point defects produced via cerium ion implantation in thin hBN flakes. We find that, to a significant fraction, emitters show bright room-temperature emission, and good optical stability suggesting the formation of Ce-based point defects. Using density functional theory (DFT) we calculate the emission properties of candidate emitters, and single out the CeVBcenter—formed by an interlayer Ce atom adjacent to a boron vacancy—as one possible microscopic model. Our results suggest an intriguing route to defect engineering that simultaneously exploits the singular properties of rare-earth ions and the versatility of two-dimensional material hosts. 
    more » « less