Abstract Chemical defects that fluoresce in the shortwave infrared open exciting opportunities in deep-penetration bioimaging, chemically specific sensing, and quantum technologies. However, the atomic size of defects and the high noise of infrared detectors have posed significant challenges to the studies of these unique emitters. Here we demonstrate high throughput single-defect spectroscopy in the shortwave infrared capable of quantitatively and spectrally resolving chemical defects at the single defect level. By cooling an InGaAs detector array down to −190 °C and implementing a nondestructive readout scheme, we are able to capture low light fluorescent events in the shortwave infrared with a signal-to-noise ratio improved by more than three orders-of-magnitude. As a demonstration, we show it is possible to resolve individual chemical defects in carbon nanotube semiconductors, simultaneously collecting a full spectrum for each defect within the entire field of view at the single defect limit.
more »
« less
Photolithographic Patterning of Organic Color‐Centers
Abstract Organic color‐centers (OCCs) have emerged as promising single‐photon emitters for solid‐state quantum technologies, chemically specific sensing, and near‐infrared bioimaging. However, these quantum light sources are currently synthesized in bulk solution, lacking the spatial control required for on‐chip integration. The ability to pattern OCCs on solid substrates with high spatial precision and molecularly defined structure is essential to interface electronics and advance their quantum applications. Herein, a lithographic generation of OCCs on solid‐state semiconducting single‐walled carbon nanotube films at spatially defined locations is presented. By using light‐driven diazoether chemistry, it is possible to directly patternp‐nitroaryl OCCs, which demonstrate chemically specific spectral signatures at programmed positions as confirmed by Raman mapping and hyperspectral photoluminescence imaging. This light‐driven technique enables the fabrication of OCC arrays on solid films that fluoresce in the shortwave infrared and presents an important step toward the direct writing of quantum emitters and other functionalities at the molecular level.
more »
« less
- PAR ID:
- 10458576
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Materials
- Volume:
- 32
- Issue:
- 14
- ISSN:
- 0935-9648
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Strong light–matter interactions in two-dimensional layered materials (2D materials) have attracted the interest of researchers from interdisciplinary fields for more than a decade now. A unique phenomenon in some 2D materials is their large exciton binding energies (BEs), increasing the likelihood of exciton survival at room temperature. It is this large BE that mediates the intense light–matter interactions of many of the 2D materials, particularly in their monolayer limit, where the interplay of excitonic phenomena poses a wealth of opportunities for high-performance optoelectronics and quantum photonics. Within quantum photonics, quantum information science (QIS) is growing rapidly, where photons are a promising platform for information processing due to their low-noise properties, excellent modal control, and long-distance propagation. A central element for QIS applications is a single photon emitter (SPE) source, where an ideal on-demand SPE emits exactly one photon at a time into a given spatiotemporal mode. Recently, 2D materials have shown practical appeal for QIS which is directly driven from their unique layered crystalline structure. This structural attribute of 2D materials facilitates their integration with optical elements more easily than the SPEs in conventional three-dimensional solid state materials, such as diamond and SiC. In this review article, we will discuss recent advances made with 2D materials towards their use as quantum emitters, where the SPE emission properties maybe modulated deterministically. The use of unique scanning tunneling microscopy tools for thein-situgeneration and characterization of defects is presented, along with theoretical first-principles frameworks and machine learning approaches to model the structure-property relationship of exciton–defect interactions within the lattice towards SPEs. Given the rapid progress made in this area, the SPEs in 2D materials are emerging as promising sources of nonclassical light emitters, well-poised to advance quantum photonics in the future.more » « less
-
Abstract A key obstacle for all quantum information science and engineering platforms is their lack of scalability. The discovery of emergent quantum phenomena and their applications in active photonic quantum technologies have been dominated by work with single atoms, self‐assembled quantum dots, or single solid‐state defects. Unfortunately, scaling these systems to many quantum nodes remains a significant challenge. Solution‐processed quantum materials are uniquely positioned to address this challenge, but the quantum properties of these materials have remained generally inferior to those of solid‐state emitters or atoms. Additionally, systematic integration of solution‐processed materials with dielectric nanophotonic structures has been rare compared to other solid‐state systems. Recent progress in synthesis processes and nanophotonic engineering, however, has demonstrated promising results, including long coherence times of emitted single photons and deterministic integration of emitters with dielectric nano‐cavities. In this review article, these recent experiments using solution‐processed quantum materials and dielectric nanophotonic structures are discussed. The progress in non‐classical light state generation, exciton‐polaritonics for quantum simulation, and spin‐physics in these materials is discussed and an outlook for this emerging research field is provided.more » « less
-
Single-photon emitters are essential in enabling several emerging applications in quantum information technology, quantum sensing, and quantum communication. Scalable photonic platforms capable of hosting intrinsic or embedded sources of single-photon emission are of particular interest for the realization of integrated quantum photonic circuits. Here, we report on the observation of room-temperature single-photon emitters in silicon nitride (SiN) films grown on silicon dioxide substrates. Photophysical analysis reveals bright (>10 5 counts/s), stable, linearly polarized, and pure quantum emitters in SiN films with a second-order autocorrelation function value at zero time delay g (2) (0) below 0.2 at room temperature. We suggest that the emission originates from a specific defect center in SiN because of the narrow wavelength distribution of the observed luminescence peak. Single-photon emitters in SiN have the potential to enable direct, scalable, and low-loss integration of quantum light sources with a well-established photonic on-chip platform.more » « less
-
Abstract The properties of a two‐level quantum dipole emitter near an ultrathin transdimensional plasmonic film are studied theoretically. The model system studied mimics a solid‐state single‐photon source device. Using realistic experimental parameters, the spontaneous and stimulated emission intensity profiles are computed as functions of the excitation frequency and film thickness, followed by the analysis of the second‐order photon correlations to explore the photon antibunching effect. It is shown that ultrathin transdimensional plasmonic films can greatly improve photon antibunching with thickness reduction, which allows one to control the quantum properties of light and make them more pronounced. Knowledge of these features is advantageous for solid‐state single‐photon source device engineering and overall for the development of the new integrated quantum photonics material platform based on the transdimensional plasmonic films.more » « less