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Viviana Villafañe

Publications and source records attributed to Viviana Villafañe.

13 recordsLinked to original sources

Temperature-Dependent Emission Spectroscopy of Quantum Emitters in Hexagonal Boron Nitride

Color centers in hexagonal boron nitride (hBN) have attracted significant interest due to their potential applications in future optical quantum technologies. For most applications, scalable on-demand fabrication is a key requirement. Recent advances using localized electron irradiation have demonstrated near-identical emitters in the blue and yellow spectral regions. While the blue emitters have been demonstrated in cryogenic temperatures, the yellow emitters remain uncharacterized under such conditions. In this work, we therefore extended the study of yellow emitters to cryogenic temperatures. Initially, multiple spectral features were observed, prompting a systematic investigation that led to the identification of a defect emission centered around 547.5 nm with high brightness and excellent photostability. By tuning the excitation wavelength, we are able to distinguish Raman scattering peaks from the emitter emission. Further analysis of the vibronic emissions allowed us to identify an optical phonon mode, whose contribution becomes increasingly dominant at elevated temperatures. Photoluminescence excitation spectroscopy (PLE) reveals excitation through this phonon mode enhances the emission by almost 5-fold in cryogenic temperature. Temperature-dependent studies further elucidate the role of phonons in the emission process. These observations deepen our understanding of the nature of the emitters, opening new avenues for precise tuning of quantum light sources.

physics.optics↗

Industry-ready spin-photon interfaces for hybrid photonic quantum computing

Hybrid photonic quantum computers, combining stationary matter qubits and flying photonic qubits, offer an intrinsically networked and resource-efficient route to large-scale, error-corrected quantum computation. Their core components are cavity-coupled matter qubits that act as light--matter interfaces, enabling: high-efficiency on-demand single-photon generation, stable near-unity photon indistinguishability and spin--multi-photon entanglement. Semiconductor quantum dots in microcavities are a leading platform for realizing such devices. Yet reaching the performance, reproducibility and spin-coherence thresholds for large-scale error correction remains a major challenge requiring industrial fabrication and control. Here we report thousands of monolithic semiconductor quantum-dot devices fabricated using a III--V pilot production-line process compatible with large-scale deployment. Systematic control of source parameters yields state-of-the-art efficiency and supports a path to optical losses below fault-tolerance thresholds. Using field-quadrature state reconstruction as a stringent joint test of efficiency and indistinguishability, we observe near-unity photon quantum purity stable over tens of minutes and a record single-photon Wigner-function negativity. We further demonstrate seven-partite spin--multi-photon entanglement and spin coherence extendable to microsecond timescales in the low-magnetic-field regime. Finally, photons from distant sources are as indistinguishable as photons emitted successively by a single source. These results establish foundry-compatible III--V quantum dots as a scalable platform for hybrid photonic quantum computing.

quant-ph↗

Mitigating the Transition of SiV$^-$ in Diamond to an Optically Dark State

Negatively charged silicon vacancy centers in diamond (SiV$^-$) are promising for quantum photonic technologies. However, when subject to resonant optical excitation, they can inadvertently transfer into a zero-spin optically dark state. We show that this unwanted change of charge state can be quickly reversed by the resonant laser itself in combination with static electric fields. By defining interdigitated metallic contacts on the diamond surface, we increase the steady-state SiV$^-$ photoluminescence under resonant excitation by a factor $\ge3$ for most emitters, making it practically constant for certain individual emitters. We electrically activate single \sivs near the positively biased electrode, which are entirely dark without applying local electric fields. Using time-resolved 3-color experiments, we show that the resonant laser not only excites the SiV$^-$, but also creates free holes that convert SiV$^{2-}$ to SiV$^-$ on a timescale of milliseconds. Through analysis of several individual emitters, our results show that the degree of electrical charge state controllability differs between individual emitters, indicating that their local environment plays a key role. Our proposed electric-field-based stabilization scheme enhances deterministic charge state control in group-IV color centers and improves its understanding, offering a scalable path toward quantum applications such as entanglement generation and quantum key distribution.

quant-ph↗

Couplings between Photons and Ensemble of Emitters in a High-$Q$ Cavity at Mesoscopic Excitation Levels

We investigate the coupling between an ensemble of individual emitters and multiple photons in a high-$Q$ cavity at the mesoscopic excitation level. The master equation theory is used to calculate the emission spectrum of the cavity QED system. The increasing excitation level not only pumps the system to the high-energy multi-emitter-photon states, but also introduces the pump-induced dephasing that suppresses the coherent energy exchange (coupling) between photons and emitters. When the emitter lifetime exceeds a threshold, we observe the mesoscopic excitation level i.e., the system is pumped to high energy states whilst the coherent couplings between these states are not yet suppressed. The mesoscopic excitation enables the couplings between multi-emitter-photon states, and thereby, paves the way to building quantum photonic devices based on multiple photons and nonlinear effects.

cond-mat.mes-hall↗

Probing Dark Excitons in Monolayer MoS$_2$ by NonLinear Two-Photon Spectroscopy

We report a new dark exciton in monolayer MoS$_2$ using second harmonic generation spectroscopy. Hereby, the spectrally dependent second harmonic generation intensity splits into two branches, and an anticrossing is observed at $\sim$ 25 meV blue detuned from the bright neutral exciton. These observations are indicative of coherent quantum interference arising from strong two-photon light-matter interaction with an excitonic state that is dark for single photon interaction. The existence of the dark state is supported by engineering its relaxation to bright localized excitons, mediated by vibrational modes of a proximal nanobeam cavity. We show that two-photon light-matter interaction involving dark states has the potential to control relaxation pathways induced by nanostructuring the local environment. Moreover, our results indicate that dark excitons have significant potential for nonlinear quantum devices based on their nontrivial excitonic photophysics.

cond-mat.mes-hall↗

Lasing of Moiré Trapped MoSe$_2$/WSe$_2$ Interlayer Excitons Coupled to a Nanocavity

We report lasing of moiré trapped interlayer excitons (IXs) by integrating a pristine hBN-encapsulated MoSe$_2$/WSe$_2$ heterobilayer into a high-$Q$ ($>10^4$) nanophotonic cavity. We control the cavity-IX detuning using a magnetic field and measure their dipolar coupling strength to be $78 \pm 4\ \mathrm{μeV}$, fully consistent with the 82 $\mathrm{μeV}$ predicted by theory. The emission from the cavity mode shows clear threshold-like behavior as the transition is tuned into resonance with the cavity. We observe a superlinear power dependence accompanied by a narrowing of the linewidth as the distinct features of lasing. The onset and prominence of these threshold-like behaviors are pronounced at resonance while weak off-resonance. Our results show that a lasing transition can be induced in interacting moiré IXs with macroscopic coherence extending over the length scale of the cavity mode. Such systems raise interesting perspectives for low-power switching and synaptic nanophotonic devices using two-dimensional materials.

cond-mat.mes-hall↗

Nonlinear Dispersion Relation and Out-of-Plane Second Harmonic Generation in MoSSe and WSSe Janus Monolayers

Janus transition metal dichalcogenides are an emerging class of atomically thin materials with engineered broken mirror symmetry that gives rise to long-lived dipolar excitons, Rashba splitting, and topologically protected solitons. They hold great promise as a versatile nonlinear optical platform due to their broadband harmonic generation tunability, ease of integration on photonic structures, and nonlinearities beyond the basal crystal plane. Here, we study second and third harmonic generation in MoSSe and WSSe Janus monolayers. We use polarization-resolved spectroscopy to map the full second-order susceptibility tensor of MoSSe, including its out-of-plane components. In addition, we measure the effective third-order susceptibility, and the second-order nonlinear dispersion close to exciton resonances for both MoSSe and WSSe at room and cryogenic temperatures. Our work sets a bedrock for understanding the nonlinear optical properties of Janus transition metal dichalcogenides and probing their use in the next-generation on-chip multifaceted photonic devices.

cond-mat.mes-hall↗

Coupling of MoS$_2$ Excitons with Lattice Phonons and Cavity Vibrational Phonons in Hybrid Nanobeam Cavities

We report resonant Raman spectroscopy of neutral excitons X$^0$ and intravalley trions X$^-$ in hBN-encapsulated MoS$_2$ monolayer embedded in a nanobeam cavity. By temperature tuning the detuning between Raman modes of MoS$_2$ lattice phonons and X$^0$/X$^-$ emission peaks, we probe the mutual coupling of excitons, lattice phonons and cavity vibrational phonons. We observe an enhancement of X$^0$-induced Raman scattering and a suppression for X$^-$-induced, and explain our findings as arising from the tripartite exciton-phonon-phonon coupling. The cavity vibrational phonons provide intermediate replica states of X$^0$ for resonance conditions in the scattering of lattice phonons, thus enhancing the Raman intensity. In contrast, the tripartite coupling involving X$^-$ is found to be much weaker, an observation explained by the geometry-dependent polarity of the electron and hole deformation potentials. Our results indicate that phononic hybridization between lattice and nanomechanical modes plays a key role in the excitonic photophysics and light-matter interaction in 2D-material nanophotonic systems.

cond-mat.mes-hall↗

Three-photon excitation of quantum two-level systems

We demonstrate that semiconductor quantum dots can be excited efficiently in a resonant three-photon process, whilst resonant two-photon excitation is highly suppressed. Time-dependent Floquet theory is used to quantify the strength of the multi-photon processes and model the experimental results. The efficiency of these transitions can be drawn directly from parity considerations in the electron and hole wavefunctions in semiconductor quantum dots. Finally, we exploit this technique to probe intrinsic properties of InGaN quantum dots. In contrast to non-resonant excitation, slow relaxation of charge carriers is avoided which allows us to measure directly the radiative lifetime of the lowest energy exciton states. Since the emission energy is detuned far from the resonant driving laser field, polarization filtering is not required and emission with a greater degree of linear polarization is observed compared to non-resonant excitation.

quant-ph↗

Emitter-Optomechanical Interaction in Ultra-High-Q hBN Nanocavities

Integrating quantum emitters into nanocavities which simultaneously couple to the photonic and mechanical modes is critical for interfacing electron spins, photons and phonons in the cavity QED system. Here, we investigate the interaction between the charged boron vacancy $V_B^-$, ultra-high-Q ($\sim10^5$) cavity photonic modes and local phonon modes. A pronounced asymmetry is observed in the emission spectrum for cavities with Q-factor above a threshold of 10$^4$. Similar asymmetries are not observed for cavities without $V_B^-$ centers. To explain our findings, we model the system with phonon-induced light-matter coupling based on $V_B^-$ centers, and compare to the Jaynes-Cummings model for usual emitters. Our results reveal that the multipartite interplay arises during the light-matter coupling of $V_B^-$ centers, illustrating that it is phonon-induced, rather than being caused by thermal population of phonon modes. Such emitter-optomechanical interaction between different photon ($V_B^-$ emission, cavity photonic) and phonon ($V_B^-$ phonon, cavity mechanical) modes provides a novel system to interface spin defects, photons and phonons in condensed matters.

cond-mat.mes-hall↗

Nonlocal Exciton-Photon Interactions in Hybrid High-Q Beam Nanocavities with Encapsulated MoS$_2$ Monolayers

Atomically thin semiconductors can be readily integrated into a wide range of nanophotonic architectures for applications in quantum photonics and novel optoelectronic devices. We report the observation of nonlocal interactions of \textit{free} trions in pristine hBN/MoS$_2$/hBN heterostructures coupled to single mode (Q $>10^4$) quasi 0D nanocavities. The high excitonic and photonic quality of the interaction system stems from our integrated nanofabrication approach simultaneously with the hBN encapsulation and the maximized local cavity field amplitude within the MoS$_2$ monolayer. We observe a nonmonotonic temperature dependence of the cavity-trion interaction strength, consistent with the nonlocal light-matter interactions in which the extent of the center-of-mass wavefunction is comparable to the cavity mode volume in space. Our approach can be generalized to other optically active 2D materials, opening the way towards harnessing novel light-matter interaction regimes for applications in quantum photonics.

cond-mat.mes-hall↗

Twist-dependent intra- and interlayer excitons in moire MoSe2 homobilayers

Optoelectronic properties of van der Waals homostructures can be selectively engineered by the relative twist angle between layers. Here, we study the twist-dependent moire coupling in MoSe2 homobilayers. For small angles, we find a pronounced redshift of the K-K and Γ-K excitons accompanied by a transition from K-K to Γ-K emission. Both effects can be traced back to the underlying moire pattern in the MoSe2 homobilayers, as confirmed by our low-energy continuum model for different moire excitons. We identify two distinct intralayer moire excitons for R-stacking, while H-stacking yields two degenerate intralayer excitons due to inversion symmetry. In both cases, bright interlayer excitons are found at higher energies. The performed calculations are in excellent agreement with experiment and allow us to characterize the observed exciton resonances, providing insight about the layer composition and relevant stacking configuration of different moire exciton species.

cond-mat.mes-hall↗

Unveiling the Zero-Phonon Line of the Boron Vacancy Center by Cavity Enhanced Emission

Negatively charged boron vacancies ($V_B^-$) in hexagonal boron nitride (hBN) exhibit a broad emission spectrum due to strong electron-phonon coupling and Jahn-Teller mixing of electronic states. As such, the direct measurement of zero-phonon line (ZPL) of $V_B^-$ has remained elusive. Here, we measure the room-temperature ZPL wavelength to be $773\pm2$ nm by coupling the hBN layer to the high-Q nanobeam cavity. As the wavelength of cavity mode is tuned, we observe a pronounced intensity resonance, indicating the coupling to $V_B^-$. Our observations are consistent with the spatial redistribution of $V_B^-$ emission. Spatially resolved measurements show a clear Purcell effect maximum at the midpoint of the nanobeam, in accord with the optical field distribution of the cavity mode. Our results are in good agreement with theoretical calculations, opening the way to using $V_B^-$ as cavity spin-photon interfaces.

cond-mat.mes-hall↗