@article{Thompson2023,
title = {Red Emission from Copper-Vacancy Color Centers in Zinc Sulfide Colloidal Nanocrystals},
author = {Sarah M. Thompson and Cüneyt Şahin and Shengsong Yang and Michael E. Flatté and Christopher B. Murray and Lee C. Bassett and Cherie R. Kagan},
url = {https://arxiv.org/abs/2301.04223},
year = {2023},
date = {2023-01-12},
abstract = {Copper-doped zinc sulfide (ZnS:Cu) exhibits down-conversion luminescence in the UV, visible, and IR regions of the electromagnetic spectrum; the visible red, green, and blue emission is referred to as R-Cu, G-Cu, and B-Cu, respectively. The sub-bandgap emission arises from optical transitions between localized electronic states created by point defects, making ZnS:Cu a prolific phosphor material and an intriguing candidate material for quantum information science, where point defects excel as single-photon sources and spin qubits. Colloidal nanocrystals (NCs) of ZnS:Cu are particularly interesting as hosts for the creation, isolation, and measurement of quantum defects, since their size, composition, and surface chemistry can be precisely tailored for bio-sensing and opto-electronic applications. Here, we present a method for synthesizing colloidal ZnS:Cu NCs that emit primarily R-Cu, which has been proposed to arise from the CuZn-VS complex, an impurity-vacancy point defect structure analogous to well-known quantum defects in other materials that produce favorable optical and spin dynamics. First principles calculations confirm the thermodynamic stability and electronic structure of CuZn-VS. Temperature- and time-dependent optical properties of ZnS:Cu NCs show blueshifting luminescence and a non-monotonic intensity dependence as temperature is increased from 19 K to 290 K, for which we propose an empirical dynamical model based on thermally-activated coupling between two manifolds of states inside the ZnS bandgap. Understanding of R-Cu emission dynamics, combined with a controlled synthesis method for obtaining R-Cu centers in colloidal NC hosts, will greatly facilitate the development of CuZn-VS and related complexes as quantum point defects in ZnS.},
keywords = {},
pubstate = {forthcoming},
tppubtype = {article}
}

@article{Narun2021,
title = {Efficient Analysis of Photoluminescence Images for the Classification of Single-Photon Emitters},
author = {Leah R. Narun and Rebecca E. K. Fishman and Henry J. Shulevitz and Raj N. Patel and Lee C. Bassett},
url = {https://pubs.acs.org/doi/10.1021/acsphotonics.2c00795
https://arxiv.org/abs/2112.05654},
doi = {10.1021/acsphotonics.2c00795},
year = {2022},
date = {2022-10-31},
journal = {ACS Photonics},
volume = {9},
number = {11},
pages = {3540–3549},
abstract = {Solid-state single-photon emitters (SPE) are a basis for emerging technologies such as quantum communication and quantum sensing. SPE based on fluorescent point defects are ubiquitous in semiconductors and insulators, and new systems with desirable properties for quantum information science may exist amongst the vast number of unexplored defects. However, the characterization of new SPE typically relies on time-consuming techniques for identifying point source emitters by eye in photoluminescence (PL) images. This manual strategy is a bottleneck for discovering new SPE, motivating a more efficient method for characterizing emitters in PL images. Here we present a quantitative method using image analysis and regression fitting to automatically identify Gaussian emitters in PL images and classify them according to their stability, shape, and intensity relative to the background. We demonstrate efficient emitter classification for SPEs in nanodiamond arrays and hexagonal boron nitride flakes. Adaptive criteria detect SPE in both samples despite variation in emitter intensity, stability, and background features. The detection criteria can be tuned for specific material systems and experimental setups to accommodate the diverse properties of SPE.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

@article{Patel2022,
title = {Probing the Optical Dynamics of Quantum Emitters in Hexagonal Boron Nitride},
author = {Raj N. Patel and David A. Hopper and Jordan A. Gusdorff and Mark E. Turiansky and Tzu-Yung Huang and Rebecca E. K. Fishman and Benjamin Porat and Chris G. Van de Walle and Lee C. Bassett},
url = {https://journals.aps.org/prxquantum/abstract/10.1103/PRXQuantum.3.030331},
doi = {10.1103/PRXQuantum.3.030331},
year = {2022},
date = {2022-09-01},
journal = {PRX Quantum},
volume = {3},
number = {3},
pages = {030331},
abstract = {Hexagonal boron nitride is a van der Waals material that hosts visible-wavelength quantum emitters at room temperature. However, experimental identification of the quantum emitters’ electronic structure is lacking, and key details of their charge and spin properties remain unknown. Here, we probe the optical dynamics of quantum emitters in hexagonal boron nitride using photon emission correlation spectroscopy. Several quantum emitters exhibit ideal single-photon emission with noise-limited photon antibunching, g(2)(0)=0. The photoluminescence emission lineshapes are consistent with individual vibronic transitions. However, polarization-resolved excitation and emission suggests the role of multiple optical transitions, and photon emission correlation spectroscopy reveals complicated optical dynamics associated with excitation and relaxation through multiple electronic excited states. We compare the experimental results to quantitative optical dynamics simulations, develop electronic structure models that are consistent with the observations, and discuss the results in the context of ab initio theoretical calculations.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

@article{Shulevitz2021,
title = {Template-Assisted Self Assembly of Fluorescent Nanodiamonds for Scalable Quantum Technologies},
author = {Henry J. Shulevitz and Tzu-Yung Huang and Jun Xu and Steven Neuhaus and Raj N. Patel and Lee C. Bassett, Cherie R. Kagan},
url = {https://arxiv.org/abs/2111.14921},
doi = {10.1021/acsnano.1c09839},
year = {2022},
date = {2022-01-13},
journal = {ACS Nano},
volume = {16},
number = {2},
pages = {1847–1856},
abstract = {Milled nanodiamonds containing nitrogen-vacancy (NV) centers provide an excellent platform for sensing applications as they are optically robust, have nanoscale quantum sensitivity, and form colloidal dispersions which enable bottom-up assembly techniques for device integration. However, variations in their size, shape, and surface chemistry limit the ability to position individual nanodiamonds and statistically study properties that affect their optical and quantum characteristics. Here, we present a scalable strategy to form ordered arrays of nanodiamonds using capillary-driven, template-assisted self assembly. This method enables the precise spatial arrangement of isolated nanodiamonds with diameters below 50 nm across millimeter-scale areas. Measurements of over 200 assembled nanodiamonds yield a statistical understanding of their structural, optical, and quantum properties. The NV centers' spin and charge properties are uncorrelated with nanodiamond size, but rather are consistent with heterogeneity in their nanoscale environment. This flexible assembly method, together with improved understanding of the material, will enable the integration of nanodiamonds into future quantum photonic and electronic devices.},
keywords = {},
pubstate = {published},
tppubtype = {article}
}

@article{Fishman2021,
title = {Photon emission correlation spectroscopy as an analytical tool for quantum defects},
author = {Rebecca E. K. Fishman and Raj N. Patel and David A. Hopper and Tzu-Yung Huang and Lee C. Bassett},
url = {https://arxiv.org/abs/2111.01252},
year = {2021},
date = {2021-11-04},
abstract = {Photon emission correlation spectroscopy has a long history in the study of atoms, molecules, and, more recently, solid-state quantum defects. In solid-state systems, its most common use is as an indicator of single-photon emission, a key property for quantum technology. However, photon correlation data can provide a wealth of information about quantum emitters beyond their single-photon purity−information that can reveal details about an emitter's electronic structure and optical dynamics that are hidden by other spectroscopy techniques. We present a standardized framework for using photon emission correlation spectroscopy to study quantum emitters, including discussion of theory, data acquisition, analysis, and interpretation. We highlight nuances and best practices regarding the commonly used g(2)(τ=0)<0.5 test for single-photon emission. Finally, we illustrate how this experimental technique can be paired with optical dynamics simulations to formulate an electronic model for unknown quantum emitters, enabling the design of quantum control protocols and assessment of their suitability for quantum information science applications.},
keywords = {},
pubstate = {forthcoming},
tppubtype = {article}
}