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Jonathan J. Finley

Publications and source records attributed to Jonathan J. Finley.

At least 37 records · Page 2Linked to original sources

Dynamically Dressed States of a Quantum Four-Level System

In this work, we experimentally and theoretically study the dressed-state emission of the biexciton-exciton cascade in a semiconductor quantum dot under pulsed, resonant, two-photon excitation. Building on the well-characterized steady-state dressed emission of the four-level system, we examine its dynamic counterpart under pulsed, resonant excitation, addressing both experimental observations and theoretical modeling. Here we report several sidebands emerging from the biexciton-to-exciton transition, whose number and spectral width depend on the excitation pulse duration and the effective pulse area, while no sidebands emerge from the exciton-to-ground-state transition. Since the biexciton state population follows a nonlinear pulse area function, sidebands with a small spectral nonlinearity result. Detuning- and time-dependent measurements provide deeper insight into the emission properties of the dressed states. They show that side peak emission only occurs in the presence of the excitation pulse. Moreover, when the system is excited by a Gaussian-shaped laser pulse, side peak emission takes place sequentially.

quant-ph↗

Resonant and Anti-resonant Exciton-Phonon Coupling in Quantum Dot Molecules

Optically active quantum dot molecules (QDMs) can host multi-spin quantum states with the potential for the deterministic generation of photonic graph states with tailored entanglement structures. Their usefulness for the generation of such non-classical states of light is determined by orbital and spin decoherence mechanisms, particularly phonon-mediated processes dominant at energy scales up to a few millielectronvolts. Here, we directly measure the spectral function of orbital phonon relaxation in a QDM and benchmark our findings against microscopic kp theory. Our results reveal phonon-mediated relaxation rates exhibiting pronounced resonances and anti-resonances, with rates ranging from several ten ns$^{-1}$ to tens of $μ$s$^{-1}$. Comparison with a kinetic model reveals the voltage (energy) dependent phonon coupling strength and fully explains the interplay between phonon-assisted relaxation and radiative recombination. These anti-resonances can be leveraged to increase the lifetime of energetically unfavorable charge configurations needed for realizing efficient spin-photon interfaces and multi-dimensional cluster states.

cond-mat.mes-hall↗

Quantum sensing with spin defects in boron nitride nanotubes

Spin defects in semiconductors are widely investigated for various applications in quantum sensing. Conventional host materials such as diamond and hexagonal boron nitride (hBN) provide bulk or low-dimensional platforms for optically addressable spin systems, but often lack the structural properties needed for chemical sensing. Here, we introduce a new class of quantum sensors based on naturally occurring spin defects in boron nitride nanotubes (BNNTs), which combine high surface area with omnidirectional spin control, key features for enhanced sensing performance. First, we present strong evidence that these defects are carbon-related, akin to recently identified centers in hBN, and demonstrate coherent spin control over ensembles embedded within dense, microscale BNNTs networks. Using dynamical decoupling, we enhance spin coherence times by a factor exceeding 300x and implement high-resolution detection of radiofrequency signals. By integrating the BNNT mesh sensor into a microfluidic platform we demonstrate chemical sensing of paramagnetic ions in solution, with detectable concentrations reaching levels nearly 1000 times lower than previously demonstrated using comparable hBN-based systems. This highly porous and flexible architecture positions BNNTs as a powerful new host material for quantum sensing.

quant-ph↗

Robust trapping of 2D excitons in an engineered 1D potential from proximal ferroelectric domain walls

We investigate the confinement of neutral excitons in a one-dimensional (1D) potential, engineered by proximizing hBN-encapsulated monolayer MoSe$_2$ to ferroelectric domain walls (DW) in periodically poled LiNbO$_3$. Our device exploits the nanometer scale in-plane electric field gradient at the DW to induce the dipolar exciton confinement via the Stark effect. Spatially resolved photoluminescence (PL) spectroscopy reveals the emergence of narrow emission lines redshifted from the MoSe$_2$ neutral exciton by up to $\sim100\,$meV, depending on the sample structure. The spatial distribution, excitation energy response and polarization properties of the emission is consistent with signatures of 1D-confined excitons. The large electric field gradients accessible via proximal ferroelectric systems open up new avenues for the creation of robust quantum-confined excitons in atomically thin materials and their heterostructures.

cond-mat.mes-hall↗

Origin of performance enhancement of superconducting nanowire single-photon detectors by He-ion irradiation

Superconducting nanowire single-photon detectors (SNSPDs) are indispensable in fields such as quantum science and technology, astronomy, and biomedical imaging, where high detection efficiency, low dark count rates and high timing accuracy are required. Recently, helium (He) ion irradiation was shown to be a promising method to enhance SNSPD performance. Here, we study how changes in the underlying superconducting NbTiN film and the SiO2/Si substrate affect device performance. While irradiated and unirradiated NbTiN films show similar crystallinity, we observe He bubble formation below the SiO2/Si interface and an amorphization of the Si substrate. Both reduce the thermal conductance between the superconducting thin film and the substrate from 210 W/m^2/K^4 to 70 W/m^2/K^4 after irradiation with 2000 ions/nm^2. This effect, combined with the lateral straggle of He ions in the substrate, allows the modification of the superconductor-to-substrate thermal conductance of an SNSPD by selectively irradiating the regions around the nanowire. With this approach, we achieved an increased plateau width of saturating intrinsic detection efficiency of 9.8 uA compared to 3.7 uA after full irradiation. Moreover, the critical current remained similar to that of the unirradiated reference device (59 uA versus 60.1 uA), while full irradiation reduced it to 22.4 uA. Our results suggest that the irradiation-induced reduction of the thermal conductance significantly enhances SNSPD sensitivity, offering a novel approach to locally engineer substrate properties for improved detector performance.

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↗

Unlocking multiphoton emission from a single-photon source through mean-field engineering

Single-photon emission from a two-level system offers promising perspectives for the development of quantum technologies, where multiphotons are generally regarded as accidental, undesired and should be suppressed. In quantum mechanics, however, multiphoton emission can turn out to be even more fundamental and interesting than the single-photon emission, since in a coherently driven system, the multiphoton suppression arises from quantum interferences between virtual multiphoton fluctuations and the mean field in a Poisson superposition of all number states. Here, we demonstrate how one can control the multiphoton dynamics of a two-level system by disrupting these quantum interferences through a precise and independent homodyne control of the mean field. We show that, counterintuitively, quantum fluctuations always play a major qualitative role, even and in fact especially, when their quantitative contribution is vanishing as compared to that of the mean field. Our findings provide new insights into the paradoxical character of quantum mechanics and open pathways for mean-field engineering as a tool for precision multiphoton control.

quant-ph↗

Competing mechanisms of dominant radiative and Auger recombination in hot carrier generation in III-V semiconductor nanowires

One-dimensional structures such as nanowires (NWs) show great promise in tailoring the rates of hot carrier thermalization in semiconductors with important implications for the design of efficient hot carrier absorbers. However, fabrication of high-quality, phase-pure crystal structures and control of their intrinsic electronic properties can be challenging, raising concerns about the role of competing radiative and non-radiative recombination mechanisms that govern hot carrier effects. Here, we elucidate the impact of crystal purity and altered electronic properties on the hot carrier properties by comparing two classes of III-V semiconductor NW arrays with similar band-gap energies and geometries, yet different crystal quality: one composed of GaAsSb NWs, free of planar stacking defects, and the other InGaAs NWs with a high density of stacking defects. Photoluminescence spectroscopy demonstrates distinct hot carrier effects in both NW arrays; however, the InGaAs NWs with lower crystal quality exhibit stronger hot carrier effects, as evidenced by increased carrier temperature under identical photoabsorptivity. This difference arises from higher rates of Auger recombination in the InGaAs NWs due to their increased n-type conductivity, as confirmed by excitation power-dependent measurements. Our findings suggest that while enhancing material properties is crucial for improving the performance of hot carrier absorbers, optimizing conditions to increase the rates of Auger recombination will further boost the efficiency of these devices.

physics.app-ph↗

Atomically Flat Dielectric Patterns for Band Gap Engineering and Lateral Junction Formation in MoSe$_2$ Monolayers

Combining a precise sputter etching method with subsequent AlO$_x$ growth within an atomic layer deposition chamber enables fabrication of atomically flat lateral patterns of SiO$_2$ and AlO$_x$. The transfer of MoSe$_2$ monolayers onto these dielectrically modulated substrates results in formation of lateral heterojunctions, with the flat substrate topography leading to minimal strain across the junction. Kelvin probe force microscopy (KPFM) measurements show significant variations in the contact potential difference (CPD) across the interface, with AlO$_x$ regions inducing a 230~mV increase in CPD. Spatially resolved photoluminescence spectroscopy reveals shifts in spectral weight of neutral and charged exciton species across the different dielectric regions. On the AlO$_x$ side, the Fermi energy moves closer to the conduction band, leading to a higher trion-to-exciton ratio, indicating a bandgap shift consistent with CPD changes. In addition, transient reflection spectroscopy highlights the influence of the dielectric environment on carrier dynamics, with the SiO$_2$ side exhibiting rapid carrier decay typical of neutral exciton recombination. In contrast, the AlO$_x$ side shows slower, mixed decay behavior consistent with conversion of trions back into excitons. These results demonstrate how dielectric substrate engineering can tune the electronic and optical characteristics of proximal two-dimensional materials, allowing scalable fabrication of advanced junctions for novel (opto)electronics applications.

cond-mat.mtrl-sci↗

Gate-tunable Bose-Fermi mixture in a strongly correlated moiré bilayer electron system

Quantum gases consisting of species with distinct quantum statistics, such as Bose-Fermi mixtures, can behave in a fundamentally different way than their unmixed constituents. This makes them an essential platform for studying emergent quantum many-body phenomena such as mediated interactions and unconventional pairing. Here, we realize an equilibrium Bose-Fermi mixture in a bilayer electron system implemented in a WS$_{2}$/WSe$_{2}$ moiré heterobilayer with strong Coulomb coupling to a nearby moiré-free WSe$_{2}$ monolayer. Absent the fermionic component, the underlying bosonic phase manifests as a dipolar excitonic insulator. By injecting excess charges into it, we show that the bosonic phase forms a stable mixture with added electrons but abruptly collapses upon hole doping. We develop a microscopic model to explain the unusual asymmetric stability with respect to electron and hole doping. By studying the Bose-Fermi mixture via monitoring excitonic resonances from both layers, we demonstrate gate-tunability over a wide range in the boson/fermion density phase space, in excellent agreement with theoretical calculations. Our results further the understanding of phases stabilized in moiré bilayer electron systems and demonstrate their potential for exploring the exotic properties of equilibrium Bose-Fermi mixtures.

cond-mat.str-el↗

Breakdown of the static dielectric screening approximation of Coulomb interactions in atomically thin semiconductors

Coulomb interactions in atomically thin materials are uniquely sensitive to variations in the dielectric screening of the environment, which can be used to control quasiparticles and exotic quantum many-body phases. A static approximation of the dielectric response, where increased dielectric screening is predicted to cause an energy redshift of the exciton resonance, has been until now sufficient. Here, we use charge-tunable exciton resonances to study screening effects in transition metal dichalcogenide monolayers embedded in materials with dielectric constants ranging from 4 to more than 1000. In contrast to expectations, we observe a blueshift of the exciton resonance exceeding 30 meV for larger dielectric constant environments. By employing a dynamical screening model, we find that while the exciton binding energy remains mostly controlled by the static dielectric response, the exciton self-energy is dominated by the high-frequency response. Dielectrics with markedly different static and high-frequency screening enable the selective addressing of distinct many-body effects in layered materials and their heterostructures, expanding the tunability range and offering new routes to detect and control correlated quantum many-body states and to design optoelectronic and quantum devices.

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↗

MBE-grown virtual substrates for quantum dots emitting in the telecom O- and C-bands

InAs semiconductor quantum dots (QDs) emitting in the near infrared are promising platforms for on-demand single-photon sources and spin-photon interfaces. However, the realization of quantum-photonic nanodevices emitting in the second and third telecom windows with similar performance remains an open challenge. Here, we report an optimized heterostructure design for QDs emitting in the O- and C-bands grown by means of molecular beam epitaxy. The InAs QDs are grown on compositionally graded InGaAs buffers, which act as virtual substrates, and are embedded in mostly relaxed active regions. Reciprocal space maps of the indium profiles and optical absorption spectra are used to optimize In0.22Ga0.78As and In0.30Ga0.70As active regions, accounting for the chosen indium grading profile. This approach results in a tunable QD photoluminescence (PL) emission from 1200 up to 1600 nm. Power and polarization dependent micro-PL measurements performed at 4 K reveal exciton-biexciton complexes from quantum dots emitting in the telecom O- and C-bands. The presented study establishes a flexible platform that can be an essential component for advanced photonic devices based on InAs/GaAs that serve as building blocks for future quantum networks.

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↗

Polarons shape the interlayer exciton emission of MoSe$_2$/WSe$_2$ heterobilayers

We present time-resolved and CW optical spectroscopy studies of interlayer excitons (IXs) in 2$H-$ and 3$R-$stacked MoSe$_2$/WSe$_2$ heterobilayers and obtain evidence for the strong participation of hot phonons in the underlying photo-physics. Photoluminescence excitation spectroscopy reveals that excess energy associated with optical excitation of \textit{intra}-layer excitons and relaxation to IXs affects the overall IX-PL lineshape, while the spectrally narrow emission lines conventionally associated with moiré IXs are unaffected. A striking uniform line-spacing of the sharp emission lines is observed together with temperature and excitation level dependent spectra suggesting an entirely new picture that photo-generated phonons lead to phonon-replicas shaping the IX-emission. Excitation power and time resolved data indicate that these features are polaronic in nature. Our experimental findings modify our current understanding of the photophysics of IXs beyond current interpretations based on moiré-trapped IXs.

cond-mat.mes-hall↗

Current-Crowding-Free Superconducting Nanowire Single-Photon Detectors

Detecting single photons is essential for applications such as dark matter detection, quantum science and technology, and biomedical imaging. Superconducting nanowire single-photon detectors (SNSPDs) excel in this task due to their near-unity detection efficiency, sub-Hz dark count rates, and picosecond timing jitter. However, a local increase of current density (current crowding) in the bends of meander-shaped SNSPDs limits these performance metrics. By locally irradiating the straight segments of SNSPDs with helium ions while leaving the bends unirradiated, we realize current-crowding-free SNSPDs with simultaneously enhanced sensitivity: after irradiation with 800 ions/nm$\unicode{xB2}$, locally irradiated SNSPDs showed a relative saturation plateau width of 37% while fully irradiated SNSPDs reached only 10%. This larger relative plateau width allows operation at lower relative bias currents, thereby reducing the dark count rate while still detecting single photons efficiently. We achieve an internal detection efficiency of 94% for a wavelength of 780 nm with a dark count rate of 7 mHz near the onset of saturating detection efficiency.

quant-ph↗

Influence of Auger heating and Shockley-Read-Hall recombination on hot carrier dynamics in InGaAs nanowires

Understanding the origin of hot carrier relaxation in nanowires (NWs) with one-dimensional (1D) geometry is significant for designing efficient hot carrier solar cells with such nanostructures. Here, we study the influence of Auger heating and Shockley-Read-Hall recombination on hot carrier dynamics of catalyst-free InGaAs-InAlAs core-shell NWs. Using steady-state and time-resolved photoluminescence (PL) spectroscopy the dependencies of hot carrier effects on the degree of confinement of photo-generated carriers induced by the nanowire diameter are determined at different lattice temperatures. Analysis of excitation-power dependent data and temperature-dependent PL linewidth broadening reveal that at low temperatures, strong Auger recombination and phonon-bottleneck are responsible for hot carrier effects. Our analysis gives also insights into electron-phonon and ionized impurity scattering, showing opposing trends with NW diameter, and it allows to estimate the Fröhlich coupling constant for the InGaAs NWs. Conversely, with increasing lattice temperature, hot carrier relaxation rates increase due to enhanced Shockley-Read Hall and surface recombination. Time-resolved spectroscopy reveals a fourfold increase in the rate of Shockley-Read-Hall recombination from 6 ns at 10 K to 1.5 ns at 150 K. The findings suggest that minimizing defect densities in the bulk and surfaces of these NWs will be key to enhance hot carrier effects towards higher temperatures.

cond-mat.mes-hall↗

Fast optoelectronic charge state conversion of silicon vacancies in diamond

Group IV vacancy color centers in diamond are promising spin-photon interfaces with strong potential for applications for photonic quantum technologies. Reliable methods for controlling and stabilizing their charge state are urgently needed for scaling to multi-qubit devices. Here, we manipulate the charge state of silicon vacancy (SiV) ensembles by combining luminescence and photo-current spectroscopy. We controllably convert the charge state between the optically active SiV$^-$ and dark SiV$^{2-}$ with MHz rates and 90% contrast by judiciously choosing the local potential applied to in-plane surface electrodes and the laser excitation wavelength. We observe intense SiV$^-$ photoluminescence under hole-capture, measure the intrinsic conversion time from the dark SiV$^{2-}$ to the bright SiV$^-$ to be 36.4(6.7)ms and demonstrate how it can be enhanced by a factor of $10^5$ via optical pumping. Moreover, we obtain new information on the defects that contribute to photo-conductivity, indicating the presence of substitutional nitrogen and divacancies.

quant-ph↗