# Strongly confined Te quantum dots as building blocks for single photon sources

Rajendra Subedi, Francisco Ruiz-Zepeda, Yagya Bahadur Woli, Thang Ba Hoang, Julien Chaste, Etienne Herth, Grégory Guisbiers

► To cite this version:

Rajendra Subedi, Francisco Ruiz-Zepeda, Yagya Bahadur Woli, Thang Ba Hoang, Julien Chaste, et al.. Strongly confined Te quantum dots as building blocks for single photon sources. Materials Today Quantum, 2025, 6, pp.100034. 10.1016/j.mtquan.2025.100034. hal-05400832

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# Strongly confined Te quantum dots as building blocks for single photon sources

Rajendra Subedi<sup>a</sup>, Francisco Ruiz-Zepeda<sup>b</sup>, Yagya Bahadur Woli<sup>c</sup>, Thang Ba Hoang<sup>c</sup>, Julien Chaste<sup>d</sup>, Etienne Herth<sup>d</sup>, Grégory Guisbiers<sup>a,*</sup>

## ARTICLE INFO

### Keywords:

Quantum dots

Tellurium

Chalcogen

Laser ablation

## ABSTRACT

Tellurium is a heavy chemical element exhibiting chirality, anisotropy, and strong spin-orbit coupling; consequently, displaying a huge potential in quantum hardware technologies. In this article, tellurium quantum dots, with sizes around 19 ± 3 nm and energy bandgap around 2.4 eV, were successfully synthesized by pulsed laser ablation in liquids (PLAL). The synthesis was performed by using a nanosecond Nd:YAG laser emitting at 1064 nm and pulsing the laser beam at 1 kHz. Toluene ($C_6H_5CH_3$) was used as a solvent to avoid oxidation of the dots. Non-polarized and polarized Raman spectroscopy as well as X-Ray diffraction were performed on the dots to study their quantum confinement and anisotropy. Finally, strongly confined tellurium quantum dots were obtained; and, their properties underline their potential as quantum light sources.

## 1. Introduction

The scientific community has shown a great interest in quantum materials [1], mainly quantum dots (QDs) since their first synthesis in the early 1980s, by Ekimov and Onushchenko [2] at the Vavilov State Optical Institute in Russia, and independently by Brus at Bell Labs in the US [3,4]. Indeed, at such scale, new opto-electronic properties emerge within the quantumly confined region [5]. This occurs when the size of the particle is below twice the value of the exciton Bohr's radius of the considered semiconductor [6,7]. Therefore, QDs are used in optoelectronic devices such as light-emitting diodes (LED) [8,9], solar cells [8, 10], photovoltaic cells [8,11], photoresistors [8], field effect transistors [8], sensors [12], and fluorescent probes [13–15]. Among all the semiconductors, Tellurium (Te) is of particular interest due to its chiral nature [16]. Indeed, Te ([Kr] 4d<sup>10</sup>5 s<sup>2</sup>5p<sup>4</sup>) has six valence electrons: two valence electrons within the 5s-orbital responsible of forming intra-chain bonds by covalent bonding; and four valence electrons within the 5p-orbital consisting of two lone-pair electrons forming inter-chain bonds by van der Waals interactions. Consequently, the crystalline structure of Te is highly anisotropic with helical chains of covalently bound atoms that are bounded together through van der

Waals interactions into a chiral hexagonal structure [17–19]. Due to its strong spin-orbit coupling (SOC), it is a promising material for new applications in optoelectronics [20–22] and spintronics [23]. In the literature, Te QDs have been synthesized by physical methods [24], chemical methods [25] and biological methods [26]. However, a major challenge is to synthesize quantum dots without capping agents. Indeed, capping agents are generally used to stop the growth of the particles at a desired size [27]. This is usually done by capping the quantum dots with a protective layer of covalently bound surfactant but this may have a detrimental effect on the optoelectronic properties of the dots. Therefore, a technique based on electrostatic repulsion rather than steric repulsion was developed [28]; that technique is known as Pulsed Laser Ablation in Liquids (PLAL). The size of nanostructures produced by PLAL can be controlled by adjusting various laser parameters such as the energy per pulse [29], repetition rate [30], fluence [31,32], wavelength [32], and by selecting the liquid medium itself [30,32] as well as the irradiation set-up [33] (bottom-ablation vs top-ablation). Due to the reactivity of Te with oxygen (O), only a very limited number of groups were able to report a successful synthesis of uncapped Te QDs by PLAL (Table 1). Indeed, the challenge during the synthesis is to avoid the oxidation of Te; that is why all the groups used an organic solvent [34,

<footnote><sup>a</sup> Department of Physics & Astronomy, University of Arkansas at Little Rock, 2801 South University Avenue, Little Rock, AR 72204, USA</footnote>

<footnote><sup>b</sup> Department of Material Chemistry, National Institute of Chemistry, 19 Hajdrihova, Ljubljana 1000, Slovenia</footnote>

<footnote><sup>c</sup> Department of Physics and Materials Science, The University of Memphis, 216 Manning Hall, Memphis, TN 38152, USA</footnote>

<footnote><sup>d</sup> Center for Nanosciences & Nanotechnologies (C2N), University of Paris-Saclay, 10 Bd Thomas Gobert, Palaiseau 91120, France</footnote>

<footnote>* Corresponding author.
E-mail address: gxguisbiers@ualr.edu (G. Guisbiers).</footnote>
<table><caption>**Table 1**
List of all the peer-reviewed papers discussing the synthesis of Te QDs by PLAL.</caption><thead><tr><th>Authors</th><th>Year</th><th>Type of laser</th><th>Wavelength (nm)</th><th>Repetition rate (Hz)</th><th>Time</th><th>Solvent</th><th>Fluence</th><th>Set-up</th></tr></thead><tbody><tr><td>Liu et al. [36]</td><td>2016</td><td>Nd:YAG</td><td>1064</td><td>10</td><td>2 s</td><td>Dichloromethane<br>CH<sub>2</sub>Cl<sub>2</sub></td><td>~6 Jcm<sup>-2</sup></td><td>Top-ablation</td></tr><tr><td>Guisbiers et al. [37]</td><td>2017</td><td>Nd:YAG</td><td>355, 532 and 1064</td><td>20</td><td>15 min</td><td>Acetone<br>(CH<sub>3</sub>)<sub>2</sub>CO</td><td>~2 Jcm<sup>-2</sup></td><td>Top-ablation</td></tr><tr><td>Novotny et al. [38]</td><td>2024</td><td>Nd:YAG</td><td>1064</td><td>10</td><td>5 min</td><td>Acetone<br>(CH<sub>3</sub>)<sub>2</sub>CO</td><td>~637 Jcm<sup>-2</sup></td><td>Top-ablation</td></tr><tr><td>This work</td><td>2025</td><td>Nd:YAG</td><td>1064</td><td>1000</td><td>5 min</td><td>Toluene<br>C<sub>6</sub>H<sub>5</sub>CH<sub>3</sub></td><td>~131 Jcm<sup>-2</sup></td><td>Bottom-ablation</td></tr></tbody></table>

<figure><img src="image_3.png" /><figcaption>**Fig. 1.** Sketch of the “Bottom-ablation” PLAL set up used to synthesize Te QDs. Insets: Bulk Te target used for irradiation (left), and colloid of Te QDs (right).</figcaption></figure>

[35]. In our case, toluene (C<sub>6</sub>H<sub>5</sub>CH<sub>3</sub>) was used. Furthermore, this manuscript is the first one to report the synthesis of strongly confined uncapped Te QDs by using a bottom-ablation PLAL setup within the kHz regime.

## 2. Materials and methods

### 2.1. Synthesis

A Q-switched Nd: YAG laser from Electro Scientific Industries emitting at 1064 nm was used to irradiate a target made of individual Te pellets (@ 99.99% from Sigma Aldrich). The pellets were placed at the bottom of the 50 ml single-neck glass flask and covered by 10 ml of toluene. The laser beam was reflected onto a flat mirror, oriented at 45° with respect to the laser rail and then focused on the surface of the target

by a bi-convex lens having a focal length of 16 mm. The lens was located between the mirror and the flask. The laser power was 12.5 W with an energy of 12.5 mJ/pulse at 1 kHz. The average beam spot size was measured to be around ~110 ± 28 µm; consequently, delivering a fluence around ~131 ± 33 Jcm<sup>-2</sup>. The target was irradiated for 5 min and immediately stored in the microtube to prevent evaporation of the solvent (Fig. 1).

### 2.2. Physico-chemical characterization

The Te QDs were characterized by Dynamic Light Scattering (DLS - NanoBrook 90Plus from Brookhaven Instruments Corporation), Transmission Electron Microscopy and Scanning Transmission Electron Microscopy (TEM and STEM- JEOL ARM 200 CF microscope operated at 80 kV), Energy Dispersive X-ray Spectrometer (EDXS- SDD JEOL Century), X-ray diffraction (XRD- Rigaku Miniflex 600 from Bruker), Raman spectroscopy (HR evolution from Horiba; laser- 532 nm), Photoluminescence (PL) spectroscopy (iHR550 from Horiba), Time-Correlated Single-Photon Counting (TCSPC) technique (PicoHarp 300 from PicoQuant), UV-visible spectroscopy (Cary 60 from Agilent) and optical microscopy (model RVL2-K4 from Echo, 20X objective lens).

For UV-visible spectroscopy and DLS analysis, 3 ml of colloid were poured into a glass cuvette for characterization. For TEM/STEM and optical microscopy, the Te QDs were dropped casted onto a TEM nickel grid and glass substrate, respectively. For X-ray diffraction analysis and Raman spectroscopy, the colloid was centrifuged @ 13,000 rpm for 1 h, using the Sorvall Legend Micro 17 from Thermo Fischer Scientific; then the sedimented particles were collected and dried into a glovebox before their analysis.

## 3. Results and discussion

The Te QDs were produced in toluene by using a bottom-ablation

<figure><img src="image_4.png" /><figcaption>**Fig. 2.** Size distribution of the Te QDs measured by a) DLS and b) TEM. Inset Figure a): photo showing on the left the toluene solvent for reference purpose only; while having on the right, the colloid containing the Te QDs. Inset Figure b): TEM image in bright field mode showing the Te QDs.</figcaption></figure>

<figure><img src="image_5.png" /></figure>
<table><caption>**Table 2**
Material properties of Te.</caption><thead><tr><th>Properties</th><th>Value</th><th>References</th></tr></thead><tbody><tr><td>Exciton Bohr's Radius, a<sub>B,ex</sub></td><td>~ 49 nm</td><td>This work</td></tr><tr><td>Electron Bohr's Radius, a<sub>B,e</sub></td><td>~ 33 nm</td><td>This work</td></tr><tr><td>Hole Bohr's Radius, a<sub>B,h</sub></td><td>~ 16 nm</td><td>This work</td></tr><tr><td>Effective mass of electron (m<sup>*</sup><sub>e</sub>)</td><td>0.055 m<sub>e</sub></td><td>[43]</td></tr><tr><td>Effective mass of hole (m<sup>*</sup><sub>h</sub>)</td><td>0.114 m<sub>e</sub></td><td>[43,44]</td></tr><tr><td>Reduced mass of exciton (m<sup>*</sup><sub>ex</sub>)</td><td>0.037 m<sub>e</sub></td><td>This work</td></tr><tr><td>Dielectric Constant (ε<sub>∞</sub>)</td><td>~ 35</td><td>This work</td></tr></tbody></table>

PLAL set-up as shown in Fig. 1. The colloid (Te QDs in toluene) displayed a grayish color as compared to the transparent color of toluene only (inset in Fig. 2a). The color is in agreement with the ones observed by all the groups listed in Table 1. By shining the beam of a red laser pointer (~ 650 nm) through the colloid, the laser light got scattered and the laser beam became visible; consequently, confirming the presence of particles within the colloid [39]. This effect is known as the “Tyndall effect”. To determine quantitatively the size of particles within the colloid, a DLS analysis was performed [40] revealing a size distribution centered around 21 ± 4 nm (Fig. 2a). Moreover, the size was also determined by electron microscopy, by performing a size analysis on TEM Bright Field images (inset Fig. 2b) with the ImageJ software. The average size of the QDs was 19 ± 3 nm as shown on Fig. 2b.

Both sizes, measured by two different techniques, DLS and TEM, were in very good agreement. To determine if the QDs were strongly confined or not, the electron's and hole's Bohr's radius had to be calculated by using their respective definition⁶ $a_{B,e} = \epsilon_{\infty} \frac{m_e}{m_e^*} a_o$ and $a_{B,h} = \epsilon_{\infty} \frac{m_h}{m_h^*} a_o$; where, $\epsilon_{\infty}$ is the dielectric constant of Te, $m_e$ is the mass of an electron 9.11 × 10⁻³¹ kg, $a_o$ is the atomic Bohr radius (0.053 nm), $m_e^*$ is the reduced mass of exciton in Te, $m_e^*$ is the effective mass of the electron in Te, $m_h^*$ is the effective mass of the hole in Te (Table 2). The electron's and hole's Bohr's radius of Te, were determined to be ~ 33 nm and ~16 nm, respectively; consequently, the exciton's Bohr radius is ~49 nm as the exciton Bohr's radius is the summation between the electron's Bohr radius and the hole's Bohr radius [6]. The value obtained in this work is in excellent agreement with the value, ~51 nm, announced by Geoffrion and Guisbiers in Refs. 6,41. Therefore, as the average size of Te QDs is smaller than twice the minimum value between the electron Bohr radius and the hole's Bohr radius; the Te QDs are strongly confined [6]. The dielectric constant value calculated in this work was determined around ~35 in excellent agreement with the value ~28 reported in Ref. 42.

The morphological study of the Te QDs was performed by TEM (Fig. 3); consequently, confirming the quasi-spherical shape of the Te QDs. Also, elemental chemical analysis was carried out by STEM-EDXS revealing solely the presence of Te within the QDs (Fig. 4).

Additionally, Raman spectroscopy was performed on the Te target (bulk sample) and on the Te QDs (Fig. 5). The Raman spectrum of the Te target exhibits three peaks (Fig. 5a): one at ~90 cm⁻¹ corresponding to the E¹ vibrational mode (bending) in which Te atoms moves along the c-axis due to an a-axis rotation; one at 120 cm⁻¹ corresponding to the A¹ vibrational mode in which each Te atom moves symmetrically into the basal plane; and one at 140 cm⁻¹ corresponding to the E² vibrational mode (stretching) in which Te atoms stretch asymmetrically along the c-axis.

<figure><img src="image_6.png" /><figcaption>**Fig. 3.** a-b) TEM bright field images of the Te QDs at different magnifications.</figcaption></figure>

<figure><img src="image_7.png" /><figcaption>**Fig. 4.** a) STEM annular dark field imaging of an agglomerate of Te QDs. b) EDXS corresponding elemental chemical map of Te QDs. The presence of Te is indicated in green.</figcaption></figure>
<figure><img src="image_8.png" /><figcaption>Fig. 5. Raman spectra of the a) bulk Te target, and b) Te QDs. Polarized Raman spectra for each vibrational mode E¹, A¹ and E² of the c) bulk Te target, and d) Te QDs.</figcaption></figure>

<figure><img src="image_9.png" /><figcaption>Fig. 6. a) XRD pattern of the bulk Te target. b) XRD pattern of Te QDs. Rigaku zero-background plate was used as sample holder to acquire the XRD spectra. The XRD peak positions were identified based on the open access database RRUFF ID: R060136. Inset: Comparison of the (101) peak position between the bulk Te target and Te QDs.</figcaption></figure>

axis (Fig. 5a) [45–50]. E¹ and E² modes are associated with intra-chains interactions while the A¹ mode is an inter-chain interaction [51]. The same vibrational modes appear in the Te QDs (Fig. 5b); while their Raman peaks underwent a blue-shift compared to the bulk Te target,

demonstrating quantum confinement [52]. By focusing on the intensity of the Raman modes, the inter-chain vibrational mode A¹ is the most intense mode followed by the intra-chain vibrational modes E² and E¹ (Fig. 4a). The same trend is observed at the quantum scale (Fig. 5b), Additionally, the anisotropy of Te was investigated by polarized Raman spectroscopy at the bulk (Fig. 5c) and quantum scale (Fig. 5d). The results obtained at the bulk scale (Fig. 5c) are in excellent agreement with Refs. 16,50. By comparing the polarized Raman spectra of the Te bulk target with the Te QDs, a slight anisotropy is still observed at the quantum scale (Figs. 5c and 5d).

The chemical composition and crystalline structure of both samples, Te target and Te QDs, were further investigated by XRD (Figs. 6a and 6b). All the XRD peaks match the hexagonal structure of Te. However, by comparing the diffraction patterns of Te QDs (Fig. 6b) with the bulk Te target (Fig. 6a), the growth orientation of Te QDs (101) did not match the one of the Te target, i.e. (202); indicating that the Te QDs were not created by fragmentation of the target, but rather by ablation. This means that the irradiated area of the Te pellet underwent melting due to the interaction of the nanosecond pulse with the target; and, then recrystallized adopting a different growth orientation. Furthermore, there is a significant decrease in intensity of the (100) peak in comparison to the (101) peak signifying a substantial anisotropy of the Te QDs (Fig. 6b); consequently, triggering a piezoelectric response as confirmed by the shift of the most intense XRD peak, the (101) peak (inset in Fig. 6b) [53]. Moreover, only Te peaks were observed in the XRD spectra confirming the purity of the QDs (Fig. 6b). By using the Scherrer equation, the crystallite size was calculated to be around 17 ± 1 nm, meaning that the Te QDs (~19 nm) were polycrystalline.

According to their preparation method, there exists two types of QDs: epitaxial and colloidal. After extensive research efforts to integrate them in optoelectronic devices, colloidal QDs appear to be a viable, tunable and low-cost solution compared to epitaxial QDs that need to be prepared under strict vacuum conditions [54,55]. Their ease of preparation triggered efforts to use them in light emitting applications. The first reports of single-photon emission from a single colloidal QD were published in 2000 by Michler et al. [56] and Lounis et al. [57]. Nowadays, colloidal QDs are commonly used as the basic building block of single photon sources [58–60]. To build a single photon source from a QD, it needs to be placed within an optical cavity. The cavity can be a Fabry-Pérot [59,61] cavity which is a typical dielectric microcavity where QDs can be easily integrated. Other types of cavity exist such as whispering gallery [62,63] and photonic crystals [64]. The integration
<figure><img src="image_10.png" /><figcaption>**Fig. 7.** a) Fluorescence image of the Te QDs. b) Tauc-plot displaying the energy bandgap of Te QDs (~2.4 eV). Inset: Absorbance spectra of the colloid. c) PL spectra of the Te QDs. d) Decay times of bulk Te (black) and Te QDs (Red).</figcaption></figure>

can be done by spin-coating, dip-coating, drop-casting, doctor blading, ink and transfer printing and imprinting [65]. After exciting the QD with a laser pulse, the cavity enhances the spontaneous emission rate of the QD due to the Purcell effect [66]. The emitted single photon is then collected using a fiber optic, and directed towards a single-photon detector. Under visible light excitation (488 nm), the Te QDs emitted light within the green region of the visible spectrum (495–570 nm) as shown in Fig. 7a. The energy bandgap of Te QDs was determined around ~2.4 eV by using the Tauc plot methodology (Fig. 7b) on the absorbance curve of Te QDs acquired by UV-visible spectroscopy (inset of Fig. 7b). Furthermore, PL spectroscopy was also performed to determine more precisely the energy bandgap of the Te QDs (Fig. 7c). Indeed, Te QDs exhibited a sharp PL emission at 498 ± 33 nm corresponding to an energy bandgap of 2.5 ± 0.2 eV. The value is identical to the one determined by UV-visible spectroscopy. The significant increase in the energy bandgap compared to the bulk value (0.33 eV) is due to quantum confinement. Additionally, time-correlated single-photon counting (TCSPC) technique was used to explore the dynamics of the photoexcited carriers within the Te QDs (Fig. 7d). The decay time of the Te QDs was compared to the one of bulk Te. From Fig. 7d, it can be seen that bulk Te curve contains one exponential and one power law component; while the QDs only contained the exponential component as mentioned by Yoshimi et al. [67]. The decay time of Te QDs and bulk Te were determined around ~2.20 ± 0.04 ns and ~0.62 ± 0.02 ns,

respectively. The longer decay time of photoexcited carriers in Te QDs is expected due to the quantum confinement effect.

By using QDs as single photon sources, biexciton are inevitably generated during the excitation, consequently emitting two photons during the biexciton relaxation; therefore, impairing the single-photon purity [68]. But the strong confinement of Te QDs enhanced the Auger effect, which is a non-radiative relaxation pathway; consequently, quenching the biexciton production and ensuring the single-photon purity [59,69].

## 4. Conclusions

In conclusion, strongly confined Te QDs were successfully synthesized for the very first time by PLAL. The size of the Te QDs was determined around 19 ± 3 nm; consequently, being within the strongly quantumly confined region for Te. Moreover, quantum confinement was experimentally confirmed by Raman spectroscopy and UV-visible spectroscopy. Indeed, the three Raman peaks of Te QDs, corresponding to the E¹, A¹ and E² modes of Te, were all blue-shifted compared to the bulk Te; and the energy bandgap of Te QDs (~2.4 eV) was about seven times larger than the bulk value of Te (~0.33 eV). Additionally, Raman spectroscopy and X-Ray diffraction analysis revealed some anisotropy for the Te QDs; consequently, suggesting a possible piezoelectric response. Finally, these strongly confined Te QDs can be used as single
photon sources in quantum technology hardware.

## Funding declaration

This work was supported by the National Science Foundation (NSF) under Grant No. 2228891, the European Research Council (ERC) Starting Grant 123STABLE (Grant No. 852208), the Agence National de la Recherche (ANR) under the FastNano project (Grant No. ANR-22-PEXD-0006), as well as the French technological network RENATECH.

## CRediT authorship contribution statement

**Subedi Rajendra:** Writing – original draft, Visualization, Investigation, Formal analysis. **Ruiz-Zepeda Francisco:** Writing – review & editing, Validation, Resources, Investigation, Formal analysis. **Woli Yagya B.:** Formal analysis, Investigation. **Hoang Thang B.:** Resources, Validation, Writing – review & editing. **Chaste Julien:** Writing – review & editing, Validation, Resources, Investigation, Formal analysis. **Herth Etienne:** Writing – review & editing, Validation, Resources, Investigation, Formal analysis. **Guisbiers Gregory:** Writing – review & editing, Visualization, Validation, Supervision, Resources, Project administration, Funding acquisition, Conceptualization.

## Declaration of Competing Interest

The authors declare the following financial interests/personal relationships which may be considered as potential competing interests: Gregory Guisbiers reports financial support was provided by National Science Foundation. Rajendra Subedi reports financial support was provided by National Science Foundation. If there are other authors, they declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

## Acknowledgments

This material is based upon research supported by the Chateaubriand Fellowship of the Office for Science & Technology of the Embassy of France in the United States.

## Data Availability

Data will be made available on request.

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