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Brian D. Gerardot

Publications and source records attributed to Brian D. Gerardot.

At least 37 records · Page 2Linked to original sources

Optical and dielectric properties of MoO$_3$ nanosheets for van der Waals heterostructures

Two-dimensional (2D) insulators are a key element in the design and fabrication of van der Waals heterostructures. They are vital as transparent dielectric spacers whose thickness can influence both the photonic, electronic, and optoelectronic properties of 2D devices. Simultaneously, they provide protection of the active layers in the heterostructure. For these critical roles, hexagonal Boron Nitride (hBN) is the dominant choice due to its large bandgap, atomic flatness, low defect density, and encapsulation properties. However, the broad catalogue of 2D insulators offers exciting opportunities to replace hBN in certain applications that require transparent thin layers with additional optical degrees of freedom. Here we investigate the potential of single-crystalline Molybdenum Oxide (MoO$_3$) as an alternative 2D insulator for the design of nanodevices that require precise adjustment of the light polarization at the nanometer scale. First, we measure the wavelength-dependent refractive indices of MoO$_3$ along its three main crystal axes and determine the in-plane and out-of-plane anisotropy of its optical properties. We find the birefringence in MoO$_3$ nanosheets compares favorably with other 2D materials that exhibit strong birefringence, such as black phosphorus, ReS$_2$, or ReSe$_2$, in particular in the visible spectral range where MoO$_3$ has the unique advantage of transparency. Finally, we demonstrate the suitability of MoO$_3$ for dielectric encapsulation by reporting linewidth narrowing and reduced inhomogeneous broadening of 2D excitons and optically active quantum emitters, respectively, in a prototypical monolayer transition-metal dichalcogenide semiconductor. These results show the potential of MoO$_3$ as a 2D dielectric layer for manipulation of the light polarization in vertical 2D heterostructures.

physics.app-ph↗

Optical dipole orientation of interlayer excitons in MoSe$_{2}$-WSe$_{2}$ heterostacks

We report on the far-field photoluminescence intensity distribution of interlayer excitons in MoSe$_{2}$-WSe$_{2}$ heterostacks as measured by back focal plane imaging in the temperature range between 1.7 K and 20 K. By comparing the data with an analytical model describing the dipolar emission pattern in a dielectric environment, we are able to obtain the relative contributions of the in- and out-of-plane transition dipole moments associated to the interlayer exciton photon emission. We determine the transition dipole moments for all observed interlayer exciton transitions to be (99 $\pm$ 1)% in-plane for R- and H-type stacking, independent of the excitation power and therefore the density of the exciton ensemble in the experimentally examined range. Finally, we discuss the limitations of the presented measurement technique to observe correlation effects in exciton ensembles.

cond-mat.mes-hall↗

Moiré-trapped interlayer trions in a charge-tunable WSe$_2$/MoSe$_2$ heterobilayer

Transition metal dichalcogenide heterobilayers offer attractive opportunities to realize lattices of interacting bosons with several degrees of freedom. Such heterobilayers can feature moiré patterns that modulate their electronic band structure, leading to spatial confinement of single interlayer excitons (IXs) that act as quantum emitters with $C_3$ symmetry. However, the narrow emission linewidths of the quantum emitters contrast with a broad ensemble IX emission observed in nominally identical heterobilayers, opening a debate regarding the origin of IX emission. Here we report the continuous evolution from a few trapped IXs to an ensemble of IXs with both triplet and singlet spin configurations in a gate-tunable $2H$-MoSe$_2$/WSe$_2$ heterobilayer. We observe signatures of dipolar interactions in the IX ensemble regime which, when combined with magneto-optical spectroscopy, reveal that the narrow quantum-dot-like and broad ensemble emission originate from IXs trapped in moiré potentials with the same atomic registry. Finally, electron doping leads to the formation of three different species of localised negative trions with contrasting spin-valley configurations, among which we observe both intervalley and intravalley IX trions with spin-triplet optical transitions. Our results identify the origin of IX emission in MoSe$_2$/WSe$_2$ heterobilayers and highlight the important role of exciton-exciton interactions and Fermi-level control in these highly tunable quantum materials.

cond-mat.mes-hall↗

Optical read-out of Coulomb staircases in a moiré superlattice via trapped interlayer trions

Moiré patterns with a superlattice potential can be formed by vertically stacking two layered materials with a relative twist or lattice constant mismatch. The moiré superlattice can generate flat bands that result in new correlated insulating, superconducting, and topological states. Strong electron correlations, tunable by the fractional filling, have been observed in both graphene and transition metal dichalcogenide (TMD) based systems. In addition, in TMD based systems, the moiré potential landscape can trap interlayer excitons (IX) at specific atomic registries. Here we report that spatially isolated trapped IX in a molybdenum diselenide/tungsten diselenide heterobilayer device provide a sensitive optical probe of carrier filling in their immediate environment. By mapping the spatial positions of individual trapped IX, we are able to spectrally track the emitters as the moiré lattice is filled with excess carriers. Upon initial doping of the heterobilayer, neutral trapped IX form charged IX (IX trions) uniformly with a binding energy of ~7 meV. Upon further doping, the empty superlattice sites sequentially fill, creating a Coulomb staircase: stepwise changes in the IX trion emission energy due to Coulomb interactions with carriers at nearest neighbour moiré sites. This non-invasive, highly local technique can complement transport and non-local optical sensing techniques to characterise Coulomb interaction energies, visualise charge correlated states, or probe local disorder in a moiré superlattice.

cond-mat.mes-hall↗

A Bright Source of Telecom Single Photons Based on Quantum Frequency Conversion

On-demand indistinguishable single photon sources are essential for quantum networking and communication. Semiconductor quantum dots are among the most promising candidates, but their typical emission wavelength renders them unsuitable for use in fibre networks. Here, we present quantum frequency conversion of near-infrared photons from a bright quantum dot to the telecommunication C-band, allowing integration with existing fibre architectures. We use a custom-built, tunable 2400 nm seed laser to convert single photons from 942 nm to 1550 nm in a difference frequency generation process. We achieve an end-to-end conversion efficiency of $\sim$35%, demonstrate count rates approaching 1 MHz at 1550 nm with $g^{\left(2\right)}\left(0\right) = 0.04$, and achieve Hong-Ou-Mandel visibilities of 60%. We expect this scheme to be preferable to quantum dot sources directly emitting at telecom wavelengths for fibre based quantum networking.

quant-ph↗

Discrete Interactions between a few Interlayer Excitons Trapped at a MoSe$_2$-WSe$_2$ Heterointerface

Interlayer excitons (IXs) in hetero-bilayers of transition metal dichalcogenides (TMDs) represent an exciting emergent class of long-lived dipolar composite bosons in an atomically thin, near-ideal two-dimensional (2D) system. The long-range interactions that arise from the spatial separation of electrons and holes can give rise to novel quantum, as well as classical multi-particle correlation effects. In order to acquire a detailed understanding of the possible many-body effects, the fundamental interactions between individual IXs have to be studied. Here, we trap a tunable number of dipolar within a nanoscale confinement potential induced by placing a MoSe$_2$-WSe$_2$ hetero-bilayer (HBL) onto an array of SiO$_2$ nanopillars. We control the mean occupation of the IX trap via the optical excitation level and observe discrete sharp-line emission from different configurations of interacting IXs. We identify these features as different multiparticle states with $N_{IX}\sim1-5$ via their power dependencies and directly measure the hierarchy of dipolar and exchange interactions as $N_{IX}$ increases. The interlayer biexciton ($N_{IX}=2$) is found to be an emission doublet that is blue-shifted from the single exciton by $ΔE=(8.4\pm0.6)$ meV and split by $2J=(1.2\pm0.5)$ meV. The blueshift is even more pronounced for triexcitons ($(12.4\pm0.4)$ meV), quadexcitons ($(15.5\pm0.6)$ meV) and quintexcitons ($(18.2\pm0.8)$ meV). These values are shown to be mutually consistent with numerical modelling of dipolar excitons confined to a harmonic trapping potential having a confinement lengthscale in the range $\ell\approx 3$ nm. Our results contribute to the understanding of interactions between IXs in TMD HBLs at the discrete limit of only a few excitations and represent a key step towards exploring quantum correlations between them.

cond-mat.mes-hall↗

Spin-layer locking of interlayer excitons trapped in moiré potentials

Van der Waals heterostructures offer attractive opportunities to design quantum materials. For instance, transition metal dichalcogenides (TMDs) possess three quantum degrees of freedom: spin, valley index, and layer index. Further, twisted TMD heterobilayers can form moiré patterns that modulate the electronic band structure according to atomic registry, leading to spatial confinement of interlayer exciton (IXs). Here we report the observation of spin-layer locking of IXs trapped in moiré potentials formed in a heterostructure of bilayer 2H-MoSe$_2$ and monolayer WSe$_2$. The phenomenon of locked electron spin and layer index leads to two quantum-confined IX species with distinct spin-layer-valley configurations. Furthermore, we observe that the atomic registries of the moiré trapping sites in the three layers are intrinsically locked together due to the 2H-type stacking characteristic of bilayer TMDs. These results identify the layer index as a useful degree of freedom to engineer tunable few-level quantum systems in two-dimensional heterostructures.

cond-mat.mes-hall↗

Resonance fluorescence from waveguide-coupled strain-localized two-dimensional quantum emitters

Efficient on-chip integration of single-photon emitters imposes a major bottleneck for applications of photonic integrated circuits in quantum technologies. Resonantly excited solid-state emitters are emerging as near-optimal quantum light sources, if not for the lack of scalability of current devices. Current integration approaches rely on cost-inefficient individual emitter placement in photonic integrated circuits, rendering applications impossible. A promising scalable platform is based on two-dimensional (2D) semiconductors. However, resonant excitation and single-photon emission of waveguide-coupled 2D emitters have proven to be elusive. Here, we show a scalable approach using a silicon nitride photonic waveguide to simultaneously strain-localize single-photon emitters from a tungsten diselenide (WSe2) monolayer and to couple them into a waveguide mode. We demonstrate the guiding of single photons in the photonic circuit by measuring second-order autocorrelation of g$^{(2)}(0)=0.150\pm0.093$ and perform on-chip resonant excitation yielding a g$^{(2)}(0)=0.377\pm0.081$. Our results are an important step to enable coherent control of quantum states and multiplexing of high-quality single photons in a scalable photonic quantum circuit.

physics.app-ph↗

Multiplexed Single Photons from Deterministically Positioned Nanowire Quantum Dots

Solid-state quantum emitters are excellent sources of on-demand indistinguishable or entangled photons and can host long-lived spin memories, crucial resources for photonic quantum information applications. However, their scalability remains an outstanding challenge. Here we present a scalable technique to multiplex streams of photons from multiple independent quantum dots, on-chip, into a fiber network for use off-chip. Multiplexing is achieved by incorporating a multi-core fiber into a confocal microscope and spatially matching the multiple foci, seven in this case, to quantum dots in an array of deterministically positioned nanowires. First, we report the coherent control of the emission of biexciton-exciton cascade from a single nanowire quantum dot under resonant two-photon excitation. Then, as a proof-of-principle demonstration, we perform parallel spectroscopy on the nanowire array to identify two nearly identical quantum dots at different positions which are subsequently tuned into resonance with an external magnetic field. Multiplexing of background-free single photons from these two quantum dots is then achieved. Our approach, applicable to all types of quantum emitters, can readily be scaled up to multiplex $>100$ quantum light sources, providing a breakthrough in hardware for photonic based quantum technologies. Immediate applications include quantum communication, quantum simulation, and quantum computation.

cond-mat.mes-hall↗

Highly tunable quantum light from moiré trapped excitons

Photon antibunching, a hallmark of quantum light, has been observed in the correlations of light from isolated atomic and atomic-like solid-state systems. Two-dimensional semiconductor heterostructures offer a unique method to create a quantum light source: a small lattice mismatch or relative twist in a heterobilayer can create moiré trapping potentials for excitons which are predicted to create arrays of quantum emitters. While signatures of moiré trapped excitons have been observed, their quantum nature has yet to be confirmed. Here we report photon antibunching from single moiré trapped interlayer excitons in a heterobilayer. Via polarization resolved magneto-optical spectroscopy, we demonstrate the discrete anharmonic spectra arise from bound band-edge electron-hole pairs trapped in moiré potentials. Finally, using an out-of-plane electric field, we exploit the large permanent dipole of interlayer excitons to achieve large DC Stark tuning, up to 40 meV, of the quantum emitters. Our results confirm the quantum nature of moiré confined excitons and open opportunities to investigate their inhomogeneity and interactions between the emitters or tune single emitters into resonance with cavity modes or other emitters.

cond-mat.mes-hall↗

Fundamental Limits to Coherent Photon Generation with Solid-State Atomlike Transitions

Coherent generation of indistinguishable single photons is crucial for many quantum communication and processing protocols. Solid-state realizations of two-level atomic transitions or three-level spin-$Λ$ systems offer significant advantages over their atomic counterparts for this purpose, albeit decoherence can arise due to environmental couplings. One popular approach to mitigate dephasing is to operate in the weak excitation limit, where excited state population is minimal and coherently scattered photons dominate over incoherent emission. Here we probe the coherence of photons produced using two-level and spin-$Λ$ solid-state systems. We observe that the coupling of the atomic-like transitions to the vibronic transitions of the crystal lattice is independent of driving strength and detuning. We apply a polaron master equation to capture the non-Markovian dynamics of the ground state vibrational manifolds. These results provide insight into the fundamental limitations for photon coherence from solid-state quantum emitters, with the consequence that deterministic single-shot quantum protocols are impossible and inherently probabilistic approaches must be embraced.

cond-mat.mes-hall↗

Out-of-plane orientation of luminescent excitons in atomically thin indium selenide flakes

Van der Waals materials offer a wide range of atomic layers with unique properties that can be easily combined to engineer novel electronic and photonic devices. A missing ingredient of the van der Waals platform is a two-dimensional crystal with naturally occurring out-of-plane luminescent dipole orientation. Here we measure the far-field photoluminescence intensity distribution of bulk InSe and two-dimensional InSe, WSe$_2$ and MoSe$_2$. We demonstrate, with the support of ab-initio calculations, that layered InSe flakes sustain luminescent excitons with an intrinsic out-of-plane orientation, in contrast with the in-plane orientation of dipoles we find in two-dimensional WSe$_2$ and MoSe$_2$ at room-temperature. These results, combined with the high tunability of the optical response and outstanding transport properties, position layered InSe as a promising semiconductor for novel optoelectronic devices, in particular for hybrid integrated photonic chips which exploit the out-of-plane dipole orientation.

cond-mat.mes-hall↗

Coulomb blockade in an atomically thin quantum dot coupled to a tunable Fermi reservoir

Gate-tunable quantum-mechanical tunnelling of particles between a quantum confined state and a nearby Fermi reservoir of delocalized states has underpinned many advances in spintronics and solid-state quantum optics. The prototypical example is a semiconductor quantum dot separated from a gated contact by a tunnel barrier. This enables Coulomb blockade, the phenomenon whereby electrons or holes can be loaded one-by-one into a quantum dot. Depending on the tunnel-coupling strength, this capability facilitates single spin quantum bits or coherent many-body interactions between the confined spin and the Fermi reservoir. Van der Waals (vdW) heterostructures, in which a wide range of unique atomic layers can easily be combined, offer novel prospects to engineer coherent quantum confined spins, tunnel barriers down to the atomic limit or a Fermi reservoir beyond the conventional flat density of states. However, gate-control of vdW nanostructures at the single particle level is needed to unlock their potential. Here we report Coulomb blockade in a vdW heterostructure consisting of a transition metal dichalcogenide quantum dot coupled to a graphene contact through an atomically thin hexagonal boron nitride (hBN) tunnel barrier. Thanks to a tunable Fermi reservoir, we can deterministically load either a single electron or a single hole into the quantum dot. We observe hybrid excitons, composed of localized quantum dot states and delocalized continuum states, arising from ultra-strong spin-conserving tunnel coupling through the atomically thin tunnel barrier. Probing the charged excitons in applied magnetic fields, we observe large gyromagnetic ratios (~8). Our results establish a foundation for engineering next-generation devices to investigate either novel regimes of Kondo physics or isolated quantum bits in a vdW heterostructure platform.

cond-mat.mes-hall↗

readPTU: a Python Library to Analyse Time Tagged Time Resolved Data

readPTU is a python package designed to analyze time-correlated single-photon counting data. The use of the library promotes the storage of the complete time arrival information of the photons and full flexibility in post-processing data for analysis. The library supports the computation of time resolved signal with external triggers and second order autocorrelation function analysis can be performed using multiple algorithms that provide the user with different trade-offs with regards to speed and accuracy. Additionally, a thresholding algorithm to perform time post-selection is also available. The library has been designed with performance and extensibility in mind to allow future users to implement support for additional file extensions and algorithms without having to deal with low level details. We demonstrate the performance of readPTU by analyzing the second-order autocorrelation function of the resonance fluorescence from a single quantum dot in a two-dimensional semiconductor.

physics.data-an↗

Atomically-thin quantum dots integrated with lithium niobate photonic chips

The electro-optic, acousto-optic and nonlinear properties of lithium niobate make it a highly versatile material platform for integrated quantum photonic circuits. A prerequisite for quantum technology applications is the ability to efficiently integrate single photon sources, and to guide the generated photons through ad-hoc circuits. Here we report the integration of quantum dots in monolayer WSe2 into a Ti in-diffused lithium niobate directional coupler. We investigate the coupling of individual quantum dots to the waveguide mode, their spatial overlap, and the overall efficiency of the hybrid-integrated photonic circuit.

physics.app-ph↗

Optimal simultaneous measurements of incompatible observables of a single photon

Joint or simultaneous measurements of non-commuting quantum observables are possible at the cost of increased unsharpness or measurement uncertainty. Many different criteria exist for defining what an "optimal" joint measurement is, with corresponding different tradeoff relations for the measurements. Understanding the limitations of such measurements is of fundamental interest and relevant for quantum technology. Here, we experimentally test a tradeoff relation for the sharpness of qubit measurements, a relation which refers directly to the form of the measurement operators, rather than to errors in estimates. We perform the first optical implementation of the simplest possible optimal joint measurement, requiring less quantum resources than have previously often been employed. Using a heralded single-photon source, we demonstrate quantum-limited performance of the scheme on single quanta.

quant-ph↗

Frequency-encoded linear cluster states with coherent Raman photons

Entangled multi-qubit states are an essential resource for quantum information and computation. Solid-state emitters can mediate interactions between subsequently emitted photons via their spin, thus offering a route towards generating entangled multi-photon states. However, existing schemes typically rely on the incoherent emission of single photons and suffer from severe practical limitations, for self-assembled quantum dots most notably the limited spin coherence time due to Overhauser magnetic field fluctuations. We here propose an alternative approach of employing spin-flip Raman scattering events of self-assembled quantum dots in Voigt geometry. We argue that weakly driven hole spins constitute a promising platform for the practical generation of frequency-entangled photonic cluster states.

quant-ph↗

Experimental triple-slit interference in a strongly-driven V-type artificial atom

Rabi oscillations of a two-level atom appear as a quantum interference effect between the amplitudes associated to atomic superpositions, in analogy with the classic double-slit experiment which manifests a sinusoidal interference pattern. By extension, through direct detection of time-resolved resonance fluorescence from a quantum-dot neutral exciton driven in the Rabi regime, we experimentally demonstrate triple-slit-type quantum interference via quantum erasure in a V-type three-level artificial atom. This result is of fundamental interest in the experimental studies of the properties of V-type 3-level systems and may pave the way for further insight into their coherence properties as well as applications for quantum information schemes. It also suggests quantum dots as candidates for multi-path-interference experiments for probing foundational concepts in quantum physics.

quant-ph↗