Nanoscale resolved mapping of the dipole emission of hBN color centers with a scattering-type scanning near-field optical microscope

Color centers in hexagonal boron nitride (hBN) are promising candidates as quantum light sources for future technologies. *

In the article “Nanoscale resolved mapping of the dipole emission of hBN color centers with a scattering-type scanning near-field optical microscope “, Iris Niehues, Daniel Wigger, Korbinian Kaltenecker, Annika Klein-Hitpass , Philippe Roell, Aleksandra K. Dąbrowska, Katarzyna Ludwiczak, Piotr Tatarczak, Janne O. Becker , Robert Schmidt, Martin Schnell, Johannes Binder, Andrzej Wysmołek and Rainer Hillenbrand utilize a scattering-type near-field optical microscope (s-SNOM) to study the photoluminescence (PL) emission characteristics of such quantum emitters in metalorganic vapor phase epitaxy grown hBN. *

On the one hand, Iris Niehues et al. demonstrate direct near-field optical excitation and emission through interaction with the nanofocus of the AFM tip resulting in a subdiffraction limited tip-enhanced PL hotspot. *

On the other hand, the authors show that indirect excitation and emission via scattering from the AFM tip significantly increases the recorded PL intensity. This demonstrates that the tip-assisted PL (TAPL) process efficiently guides the generated light to the detector. *

Iris Niehues et al. apply the TAPL method to map the in-plane dipole orientations of the hBN color centers on the nanoscale. This work promotes the widely available s-SNOM approach to applications in the quantum domain including characterization and optical control. *

The investigation utilizes a scattering-type near-field optical microscope employing a metallized Arrow AFM tip ( NanoWorld Arrow-NCPt AFM probe) illuminated by monochromatic laser light. *

The AFM tip acts as an optical antenna, transforming the incident p-polarizedlight into a highly focused near field at the AFM tip apex, the so-called nanofocus. *

The nanofocus interacts with the sample leading to modified scattering from the AFM tip and encoding local sample properties.

In conventional s-SNOM operation, the elastically scattered light is recorded as function of sample position (note that the sample is scanned), yielding near-field optical images with a spatial resolution down to 10 nm. *

To supress background scattering, the AFM is operated in tapping mode and the detector signal is demodulated at a higher harmonic of the AFM tip’s oscillation frequency. *

In the article, Iris Niehues et al. use the s-SNOM instrument to study PL from individual hBN color centers. *

To that end, the inelastically tip-scattered light is recorded with a grating spectrometer coupled to a CCD camera. Note that signal demodulation has not been possible with the use of a CCD camera so far. It may be achieved employing a photomultiplier tube or similar. Importantly, the authors’ s-SNOM setup includes a high-quality, silver-protected off-axis parabolic mirror with a numerical aperture (NA) of 0.72, which optimizes the focusing and collection efficiency of the optical system and is crucial for the performed PL measurements. *

Characterization of photoluminescence mapping

In the specific experiments performed by “, Iris Niehues et al., the authors employ the near-field optical microscope in tapping mode, with low oscillation amplitudes between 20 nm and 30 nm, to detect PL signals influenced by the presence of the metallic AFM tip. *

They use standard metallic Arrow AFM tips (NanoWorld Arrow-NCPt) Throughout this study, Iris Niehues et al., use a 532 nm (2.33 eV) laser for the optical excitation of the hBN color centers. *

Figure 1 from Iris Niehues et al. 2025 “Nanoscale resolved mapping of the dipole emission of hBN color centers with a scattering-type scanning near-field optical microscope” :Photoluminescence (PL) measurement of a single color center taken with an AFM tip. The images are shown with the same color bar for better comparison of the observed PL intensities. (a) PL intensity map without the tip showing a diffraction limited emission spot. (b) PL spectrum of the studied emitter recorded with an extended integration time inside the arc in (c). The zero-phonon line (ZPL) and optical phonon sidebands (PSBs) of 160 meV are marked as well as the broad background PL (black line). (c) PL map of the same emitter with the AFM tip showing two subdiffraction limit features marked as “dot” and “arc.” (d) Lineprofiles along the dashed lines in (a) in black and (c) in red (dark measurement, bright Gaussian fits). The fitted full widths at half maximum (FWHM) are 110 nm (dot), 209 nm (arc), and 1,418 nm (w/o tip). (e) Schematic of the interference between direct and indirect excitation/emission of the color center via the AFM tip (TAPL). Inset shows the nanofocus interaction at the location of the color center explaining the dot (TEPL). (f) Analytical reproduction of the TAPL arc in (c) applying the model in (e). NanoWorld Arrow-NCPt AFM probes with a platinum iridium coating were used.
Figure 1 from Iris Niehues et al. 2025 “Nanoscale resolved mapping of the dipole emission of hBN color centers with a scattering-type scanning near-field optical microscope” :
Photoluminescence (PL) measurement of a single color center taken with an AFM tip. The images are shown with the same color bar for better comparison of the observed PL intensities. (a) PL intensity map without the tip showing a diffraction limited emission spot. (b) PL spectrum of the studied emitter recorded with an extended integration time inside the arc in (c). The zero-phonon line (ZPL) and optical phonon sidebands (PSBs) of 160 meV are marked as well as the broad background PL (black line). (c) PL map of the same emitter with the AFM tip showing two subdiffraction limit features marked as “dot” and “arc.” (d) Lineprofiles along the dashed lines in (a) in black and (c) in red (dark measurement, bright Gaussian fits). The fitted full widths at half maximum (FWHM) are 110 nm (dot), 209 nm (arc), and 1,418 nm (w/o tip). (e) Schematic of the interference between direct and indirect excitation/emission of the color center via the AFM tip (TAPL). Inset shows the nanofocus interaction at the location of the color center explaining the dot (TEPL). (f) Analytical reproduction of the TAPL arc in (c) applying the model in (e).

*Iris Niehues, Daniel Wigger, Korbinian Kaltenecker, Annika Klein-Hitpass , Philippe Roell, Aleksandra K. Dąbrowska, Katarzyna Ludwiczak, Piotr Tatarczak, Janne O. Becker , Robert Schmidt, Martin Schnell, Johannes Binder, Andrzej Wysmołek and Rainer Hillenbrand
Nanoscale resolved mapping of the dipole emission of hBN color centers with a scattering-type scanning near-field optical microscope
Nanophotonics, vol. 14, no. 3, 2025, pp. 335-342
DOI: https://doi.org/10.1515/nanoph-2024-0554

Open Access  The article “Nanoscale resolved mapping of the dipole emission of hBN color centers with a scattering-type scanning near-field optical microscope” by Iris Niehues, Daniel Wigger, Korbinian Kaltenecker, Annika Klein-Hitpass , Philippe Roell, Aleksandra K. Dąbrowska, Katarzyna Ludwiczak, Piotr Tatarczak, Janne O. Becker , Robert Schmidt, Martin Schnell, Johannes Binder, Andrzej Wysmołek and Rainer Hillenbrand is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/.

Highly efficient carbon-dot-based photoinitiating systems for 3D-VAT printing

Known as a rising star among carbon nanomaterials, carbon dots (CDs) have attracted considerable interest in various fields in recent years.*

In the article “Highly efficient carbon dot-based photoinitiating systems for 3D-VAT printing” Dominika Krok, Wiktoria Tomal, Alexander J. Knight, Alexander I. Tartakovskii, Nicholas T. H. Farr, Wiktor Kasprzyk and Joanna Ortyl describe how they synthesized different types of carbon dots (CDs) based on citric acid as a precursor using an efficient procedure to purify these materials from low molecular by-products and fluorophores.*

They introduce three types of CDs: citric acid-based, as well as ammonia- and ethylenediamine-doped CDs, and compare their effectiveness to commercially available graphene-based CDs as an element of two- or three-component photoinitiating systems dedicated for free radical photopolymerization processes.*

This approach led to the development of efficient initiating systems and allowed better understanding of the mechanism according to which CDs performed in these processes. *

As the proof of concept, CDs-based photoinitiating systems were implemented in two types of 3D-VAT printing processes: DLP and DLW printing, to obtain high-resolution, 3D hydrogel materials. *

Dominika Krok et al. believe that the research presented in their article will become the basis for further work on carbon dots in the context of the diverse use of photopolymerization processes and avoid errors affecting the misinterpretation of data. *

The morphology and chemical composition of obtained hydrogel printouts were profoundly characterized via scanning electron microscopy (SEM), atomic force microscopy (AFM), nanoscale Fourier transform infrared spectroscopy (Nano-FTIR), and scattering-type Scanning Near-field Optical Microscopy (s-SNOM). *

The s-SNOM system used to collect the data shown in figure 12 of the article cited below, consisted of an AFM within one arm of an interferometer, and a moveable mirror in the other. *

A conductive platinum-iridium coated NanoWorld ARROW-EFM AFM probe was brought into tapping mode operation upon the sample (tapping frequency 77 kHz, tapping amplitude 71 nm), and illumination from a single-wavelength source outputting at 1490 cm−1 was sent into the interferometer. *

Under focused illumination, the conductive AFM tip acts as an optical antenna and a near field is generated at the AFM tip apex (AFM tip radius around 25 nm). The near field interacts with the sample surface and forms a scattering centre that scatters further incoming photons. *

The scattered photons were collected at the detector and interfered with photons returning from the movable mirror in the reference arm of the interferometer. This reference mirror was oscillated in order to induce side-band frequency mixing in the optical signal power spectrum, and the optical amplitude and phase data were extracted at the third harmonic of the AFM tapping frequency. *

The optical amplitude data were normalised to the maximum recorded value. The optical phase data were left unprocessed, and thus the raw values of the phase data in Fig. 12 (cited below) do not hold physical meaning. Only the contrast between two areas of Fig. 12 should be considered. *

AFM data: AFM topology data were recorded using the same instrument as used for the s-SNOM measurements. Conductive AFM cantilevers (Pt/Ir coated ARROW-EFM AFM probes from NanoWorld) were used, at a tapping frequency of 77 kHz and a tapping amplitude of 71 nm. *

Further surface characterization of the hydrogel samples performed with AFM and s-SNOM techniques revealed that, occasionally, carbon dot particles can be found at or emerging from the surface of the hydrogel.  *

Fig. 12D presents the surface topography of an 8 μm by 6.8 μm region of hydrogel as measured through AFM, which is in keeping with the surface characterization data presented in Fig. 12A–C. It is not obvious from the topography data in Fig. 12D alone which features of the sample surface relate to carbon material. *

However, the carbon dot particles can be identified through the mechanical properties of their surface: Fig. 15E in the cited article presents the AFM phase data from the scan shown in Fig. 12D, with AFM phase being sensitive to various mechanical surface properties of the sample material such as hardness and adhesion. *

A strong phase contrast is observed between the soft hydrogel and the harder carbon dot material, allowing for the identification of a carbon dot particle that is only partially covered by the hydrogel. *

Additionally, Fig. 12F presents s-SNOM optical phase data taken during the scan shown in Fig. 12D, using illumination at 1490 cm−1. s-SNOM measurements are sensitive to optical properties such as refractive index and absorption, and the differences in these properties between the hydrogel and carbon dot materials creates strong contrast in s-SNOM phase data, allowing for further verification of the location of the carbon dot particle. *

Dominika Krok et al. note that often large areas of the hydrogel surface had to be scanned before any carbon dot particles partially above the surface were identified, and that no carbon dot particles were found either entirely or mostly above the surface of the hydrogel. *

It is therefore assumed that the CDs embedded within the 3D-VAT prints do not congregate on the surface of the material but instead are distributed throughout the matrix. *

Fig. 12 from “Highly efficient carbon dot-based photoinitiating systems for 3D-VAT printing” by Dominika Krok et al. (2023):(A) Low magnification secondary electron (SE) image of a 3D-VAT printout taken using an Everhart–Thornley Detector (ETD). (B) High resolution SE image of a 3D-VAT printout taken using a Through Lens Detector (TLD). (C) Backscattered election (BSE) image taken using a concentric backscatter (CBS) detector. (D): AFM height topography of a carbon dot at the surface of a hydrogel sample. (E) AFM mechanical phase data taken simultaneously with the data in (D). AFM phase data is sensitive to a number of surface properties (hardness, adhesion, etc.) and is often difficult to interpret. In this case, we simply note that the AFM phase contrast observed in (E) allows for easy distinction between areas of the hydrogel (high AFM phase) and the carbon dot surface (low AFM phase). (F): s-SNOM phase data taken simultaneously with the data in (D), with incident illumination at 1490 cm−1. The s-SNOM data was demodulated at the 3rd harmonic of the AFM tapping frequency to reduce the influence of background effects. The hydrogel and the carbon dot particle have different optical responses under the incident illumination, and so s-SNOM phase contrast is observed between the different regions of the AFM scan. Corresponding s-SNOM amplitude data is shown in Fig. S22 of the ESI.† The s-SNOM system used to collect the data shown in this figure consisted of an AFM within one arm of an interferometer, and a moveable mirror in the other. * A conductive platinum-iridium coated NanoWorld ARROW-EFM AFM probe was brought into tapping mode operation upon the sample (tapping frequency 77 kHz, tapping amplitude 71 nm), and illumination from a single-wavelength source outputting at 1490 cm−1 was sent into the interferometer. *
Fig. 12 from “Highly efficient carbon dot-based photoinitiating systems for 3D-VAT printing” by Dominika Krok et al. (2023):
(A) Low magnification secondary electron (SE) image of a 3D-VAT printout taken using an Everhart–Thornley Detector (ETD). (B) High resolution SE image of a 3D-VAT printout taken using a Through Lens Detector (TLD). (C) Backscattered election (BSE) image taken using a concentric backscatter (CBS) detector. (D): AFM height topography of a carbon dot at the surface of a hydrogel sample. (E) AFM mechanical phase data taken simultaneously with the data in (D). AFM phase data is sensitive to a number of surface properties (hardness, adhesion, etc.) and is often difficult to interpret. In this case, we simply note that the AFM phase contrast observed in (E) allows for easy distinction between areas of the hydrogel (high AFM phase) and the carbon dot surface (low AFM phase). (F): s-SNOM phase data taken simultaneously with the data in (D), with incident illumination at 1490 cm−1. The s-SNOM data was demodulated at the 3rd harmonic of the AFM tapping frequency to reduce the influence of background effects. The hydrogel and the carbon dot particle have different optical responses under the incident illumination, and so s-SNOM phase contrast is observed between the different regions of the AFM scan. Corresponding s-SNOM amplitude data is shown in Fig. S22 of the ESI.†

*Dominika Krok, Wiktoria Tomal, Alexander J. Knight, Alexander I. Tartakovskii, Nicholas T. H. Farr, Wiktor Kasprzyk and Joanna Ortyl
Highly efficient carbon dot-based photoinitiating systems for 3D-VAT printing
Polymer Chemistry, 2023, 14, 4429-4444
DOI:  https://doi.org/10.1039/D3PY00726J

The article “Highly efficient carbon dot-based photoinitiating systems for 3D-VAT printing” by Dominika Krok, Wiktoria Tomal, Alexander J. Knight, Alexander I. Tartakovskii, Nicholas T. H. Farr, Wiktor Kasprzyk and Joanna Ortyl is licensed under a Creative Commons Attribution 3.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third-party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit https://creativecommons.org/licenses/by/3.0/.

Manipulating hyperbolic transient plasmons in a layered semiconductor

Anisotropic materials with oppositely signed dielectric tensors support hyperbolic polaritons, displaying enhanced electromagnetic localization and directional energy flow. *

However, the most reported hyperbolic phonon polaritons are difficult to apply for active electro-optical modulations and optoelectronic devices. *

In the nature communications letter “Manipulating hyperbolic transient plasmons in a layered semiconductor”, Rao Fu, Yusong Qu, Mengfei Xue, Xinghui Liu, Shengyao Chen, Yongqian Zhao, Runkun Chen, Boxuan Li, Hongming Weng, Qian Liu, Qing Dai and Jianing Chen report a dynamic topological plasmonic dispersion transition in black phosphorus (BP) via photo-induced carrier injection, i.e., transforming the iso-frequency contour from a pristine ellipsoid to a non-equilibrium hyperboloid. *

They introduce a promising approach to optically manipulate robust transient hyperbolic plasmons in the layered semiconductor black phosphorus using a dedicated ultrafast nanoscopy scheme. Optical pumping allows the BP’s IFCs to topologically transit from the pristine ellipsoid to the non-equilibrium hyperboloid, exhibiting exotic non-equilibrium hyperbolic plasmon properties, such as the optically tunable plasmonic dispersion and the coexistence of different transient plasmonic modes. *

Their work also demonstrates the peculiar transient plasmonic properties of the studied layered semiconductor, such as the ultrafast transition, low propagation losses, efficient optical emission from the black phosphorus’s edges, and the characterization of different transient plasmon modes. *

The results that Rao Fu et al. present may be relevant for the development of future optoelectronic applications. *

NanoWorld® ARROW-NCPt AFM probes with a Pt/Ir coating were used for the characterization with ultrafast nanoscopy. The pump and probe pulses were spatially overlapped on the Platinum/Iridium coated Arrow probe through a parabolic mirror of a commercial scattering-type scanning near-field optical microscope. *

Fig. 4 from Rao Fu et al. “Manipulating hyperbolic transient plasmons in a layered semiconductor”:Dynamic analysis of the transient plasmons. a Normalized near-field amplitude s3/s3,Si of a 280-nm-thick BP slab for twelve delay times τ. Scale bar, 1 µm. b Near-field amplitude curves for the corresponding twelve different delay times τ in a. c Dynamics of the relative near-field intensity of the first (∆S1) and the second bright strip (∆S2) in b. Opened circles are the experimental data, and solid lines are bi-exponential fitting for ∆S1 and exponential fitting for ∆S2, respectively. d Dynamics of the near-field amplitude s3 from the black circle in a. The inset displays the s3 at τ = −2 to 6 ps, and the dashed line marks the s3 level of the pristine state. NanoWorld® ARROW-NCPt AFM probes with a Pt/Ir coating were used for the characterization with ultrafast nanoscopy. The pump and probe pulses were spatially overlapped on the Pt/Ir coated Arrow probe through a parabolic mirror of a commercial scattering-type scanning near-field optical microscope.
Fig. 4 from Rao Fu et al. “Manipulating hyperbolic transient plasmons in a layered semiconductor”:
Dynamic analysis of the transient plasmons.
a Normalized near-field amplitude s3/s3,Si of a 280-nm-thick BP slab for twelve delay times τ. Scale bar, 1 µm. b Near-field amplitude curves for the corresponding twelve different delay times τ in a. c Dynamics of the relative near-field intensity of the first (∆S1) and the second bright strip (∆S2) in b. Opened circles are the experimental data, and solid lines are bi-exponential fitting for ∆S1 and exponential fitting for ∆S2, respectively. d Dynamics of the near-field amplitude s3 from the black circle in a. The inset displays the s3 at τ = −2 to 6 ps, and the dashed line marks the s3 level of the pristine state.

*Rao Fu, Yusong Qu, Mengfei Xue, Xinghui Liu, Shengyao Chen, Yongqian Zhao, Runkun Chen, Boxuan Li, Hongming Weng, Qian Liu, Qing Dai and Jianing Chen
Manipulating hyperbolic transient plasmons in a layered semiconductor

Nature Communications volume 15, Article number: 709 (2024)
DOI: https://doi.org/10.1038/s41467-024-44971-3

Please follow this external link to read the full article: https://rdcu.be/dBD85

The article “Manipulating hyperbolic transient plasmons in a layered semiconductor” by Rao Fu, Yusong Qu, Mengfei Xue, Xinghui Liu, Shengyao Chen, Yongqian Zhao, Runkun Chen, Boxuan Li, Hongming Weng, Qian Liu, Qing Dai and Jianing Chen is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third-party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit https://creativecommons.org/licenses/by/4.0/.