arXiv subjects

B. D. Gerardot

Publications and source records attributed to B. D. Gerardot.

At least 19 recordsLinked to original sources

arXiv2025

Photoexcitation of moiré-trapped interlayer excitons via chiral phonons

Moiré superlattices in transition-metal dichalcogenide semiconductor heterobilayers enable the quantum confinement of interlayer excitons with large out-of-plane permanent electric dipoles and spin-valley control. Here, we report a novel phonon-assisted excitation mechanism of individual moiré-trapped interlayer excitons in 2H-stacked MoSe$_2$/WSe$_2$ heterobilayers via chiral $E^{\prime\prime}$ in-plane optical phonons at the Γ-point. This excitation pathway preserves valley-selective optical selection rules and enables deterministic generation of individual interlayer excitons with defined helicity, emitting within a spectrally narrow energy spread. Through photoluminescence excitation spectroscopy in both the ensemble and quantum emitter regimes, we identify a fixed phonon energy of $\sim$23 meV mediating the process. First-principles calculations corroborate the symmetry and energy of the relevant phonon mode and its coupling to interlayer excitons, providing microscopic support for the observed valley-selective phonon-assisted excitation mechanism. Our results highlight the utility of chiral phonons as a tool for controlled excitation of quantum emitters in TMD moiré systems, opening new opportunities for valleytronic and quantum photonic applications.

quant-ph↗

arXiv2022

Moiré straintronics: a universal platform for reconfigurable quantum materials

Large scale two-dimensional (2D) moiré superlattices are driving a revolution in designer quantum materials. The electronic interactions in these superlattices, strongly dependent on the periodicity and symmetry of the moiré pattern, critically determine the emergent properties and phase diagrams. To date, the relative twist angle between two layers has been the primary tuning parameter for a given choice of constituent crystals. Here, we establish strain as a powerful mechanism to in-situ modify the moiré periodicity and symmetry. We develop an analytically exact mathematical description for the moiré lattice under arbitrary in-plane heterostrain acting on any bilayer structure. We demonstrate the ability to fine-tune the moiré lattice near critical points, such as the magic angle in bilayer graphene, or fully reconfigure the moiré lattice symmetry beyond that imposed by the unstrained constituent crystals. Due to this unprecedented simultaneous control over the strength of electronic interactions and lattice symmetry, 2D heterostrain provides a powerful platform to engineer, tune, and probe strongly correlated moiré materials.

cond-mat.mes-hall↗

arXiv2020

Coherent Dynamics in Quantum Emitters under Dichromatic Excitation

We characterize the coherent dynamics of a two-level quantum emitter driven by a pair of symmetrically-detuned phase-locked pulses. The promise of dichromatic excitation is to spectrally isolate the excitation laser from the quantum emission, enabling background-free photon extraction from the emitter. Paradoxically, we find that excitation is not possible without spectral overlap between the exciting pulse and the quantum emitter transition for ideal two-level systems due to cancellation of the accumulated pulse area. However, any additional interactions that interfere with cancellation of the accumulated pulse area may lead to a finite stationary population inversion. Our spectroscopic results of a solid-state two-level system show that while coupling to lattice vibrations helps to improve the inversion efficiency up to 50\% under symmetric driving, coherent population control and a larger amount of inversion are possible using asymmetric dichromatic excitation, which we achieve by adjusting the ratio of the intensities between the red and blue-detuned pulses. Our measured results, supported by simulations using a real-time path-integral method, offer a new perspective towards realising efficient, background-free photon generation and extraction.

quant-ph↗

arXiv2019

Monolithic semiconductor hemispherical micro cavities for efficient single photon extraction

We present a monolithic semiconductor microcavity design for enhanced light-matter interaction and photon extraction efficiency of an embedded quantum emitter such as a quantum dot or color center. The microcavity is a hemispherical Fabry-Perot design consisting of a planar back mirror and a top curved mirror. Higher order modes are suppressed in the structure by reducing the height of the curved mirror, leading to efficient photon extraction into a fundamental mode with a Gaussian far-field radiation pattern. The cavity finesse can be varied easily by changing the reflectivity of the mirrors and we consider two specific cases: a low-finesse structure for enhanced broad band photon extraction from self-assembled quantum dots and a moderate-finesse cavity for enhanced extraction of single photons from the zero-phonon line of color centers in diamond. We also consider the impact of structural imperfections on the cavity performance. Finally, we present the fabrication and optical characterisation of monolithic GaAs hemispherical microcavities.

physics.app-ph↗

arXiv2018

Microcavity enhanced single photon emission from two-dimensional WSe2

Atomically flat semiconducting materials such as monolayer WSe$_2$ hold great promise for novel optoelectronic devices. Recently, quantum light emission has been observed from bound excitons in exfoliated WSe$_2$. As part of developing optoelectronic devices, the control of the radiative properties of such emitters is an important step. Here we report the coupling of a bound exciton in WSe$_2$ to open microcavities. We use a range of radii of curvature in the plano-concave cavity geometry with mode volumes in the $λ^3$ regime, giving Purcell factors of up to 8 while increasing the photon flux five-fold. Additionally we determine the quantum efficiency of the single photon emitter to be $η= 0.46 \pm 0.03$. Our findings pave the way to cavity-enhanced monolayer based single photon sources for a wide range of applications in nanophotonics and quantum information technologies.

cond-mat.mes-hall↗

arXiv2016

Resonance fluorescence from a telecom-wavelength quantum dot

We report on resonance fluorescence from a single quantum dot emitting at telecom wavelengths. We perform high-resolution spectroscopy and observe the Mollow triplet in the Rabi regime--a hallmark of resonance fluorescence. The measured resonance-fluorescence spectra allow us to rule out pure dephasing as a significant decoherence mechanism in these quantum dots. Combined with numerical simulations, the experimental results provide robust characterisation of charge noise in the environment of the quantum dot. Resonant control of the quantum dot opens up new possibilities for on-demand generation of indistinguishable single photons at telecom wavelengths as well as quantum optics experiments and direct manipulation of solid-state qubits in telecom-wavelength quantum dots.

cond-mat.mes-hall↗

arXiv2016

Resonance fluorescence and laser spectroscopy of three-dimensionally confined excitons in monolayer WSe$_2$

Resonant optical excitation of few-level quantum systems enables coherent quantum control, resonance fluorescence, and direct characterization of dephasing mechanisms. Experimental demonstrations have been achieved in a variety of atomic and solid-state systems. An alternative but intriguing quantum photonic platform is based on single layer transition metal chalcogenide semiconductors, which exhibit a direct band-gap with optically addressable exciton valley-pseudospins in a uniquely two-dimensional form. Here we perform resonance and near-resonance excitation of three-dimensionally confined excitons in monolayer WSe$_2$ to reveal near ideal single photon fluorescence with count rates up to 3 MHz and uncover a weakly-fluorescent exciton state ~ 5 meV blue-shifted from the ground-state exciton. We perform high-resolution photoluminescence excitation spectroscopy of the localized excitons, providing important information to unravel the precise nature of the quantum states. Successful demonstration of resonance fluorescence paves the way to probe the localized exciton coherence. Moreover, these results yield a route for investigations of the spin and valley coherence of confined excitons in two-dimensional semiconductors.

cond-mat.mes-hall↗

arXiv2016

Screening nuclear field fluctuations in quantum dots for indistinguishable photon generation

A semiconductor quantum dot can generate highly coherent and indistinguishable single photons. However, intrinsic semiconductor dephasing mechanisms can reduce the visibility of two-photon interference. For an electron in a quantum dot, a fundamental dephasing process is the hyperfine interaction with the nuclear spin bath. Here we directly probe the consequence of the fluctuating nuclear spins on the elastic and inelastic scattered photon spectra from a resident electron in a single dot. We find the nuclear spin fluctuations lead to detuned Raman scattered photons which are distinguishable from both the elastic and incoherent components of the resonance fluorescence. This significantly reduces two-photon interference visibility. However, we demonstrate successful screening of the nuclear spin noise which enables the generation of coherent single photons that exhibit high visibility two-photon interference.

cond-mat.mes-hall↗

arXiv2014

A strain-tunable quantum dot embedded in a nanowire antenna

We demonstrate an elastically-tunable self-assembled quantum dot in a nanowire antenna that emits single photons with resolution-limited spectral linewidths. The single-photon device is comprised of a single quantum dot embedded in a top-down fabricated nanowire waveguide integrated onto a piezoelectric actuator. Non-resonant excitation leads to static (fluctuating) charges likely at the nanowire surface, causing DC Stark shifts (inhomogeneous broadening); for low excitation powers, the effects are not observed and resolution-limited linewidths are obtained. Despite significant strain-field relaxation in the high-aspect-ratio nanowires, we achieve up to 1.2 meV tuning of a dot's transition energy. Single-photon sources with high brightness, resolution-limited linewidths, and wavelength tunability are promising for future quantum technologies.

cond-mat.mes-hall↗

arXiv2011

Probing single charge fluctuations in a semiconductor with laser spectroscopy on a quantum dot

We probe local charge fluctuations in a semiconductor via laser spectroscopy on a nearby self-assembled quantum dot. We demonstrate that the quantum dot is sensitive to changes in the local environment at the single charge level. By controlling the charge state of localized defects, we are able to infer the distance of the defects from the quantum dot with +-5 nm resolution. The results identify and quantify the main source of charge noise in the commonly-used optical field-effect devices. Based on this understanding we achieve routinely close-totransform-limited quantum dot optical linewidths.

cond-mat.mes-hall↗

arXiv2011

Laser spectroscopy of individual quantum dots charged with a single hole

We characterize the positively charged exciton (X1+) in single InGaAs quantum dots using resonant laser spectroscopy. Three samples with different dopant species (Be or C as acceptors, Si as a donor) are compared. The p-doped samples exhibit larger inhomogeneous broadening (x3) and smaller absorption contrast (x10) than the n-doped sample. For X1+ in the Be-doped sample, a dot dependent non-linear Fano effect is observed, demonstrating coupling to degenerate continuum states. However, for the C-doped sample the X1+ lineshape and saturation broadening follows isolated atomic transition behaviour. This C-doped device structure is useful for single hole spin initialization, manipulation, and measurement.

cond-mat.mes-hall↗

arXiv2011

Controlling the Interaction of Electron and Nuclear Spins in a Tunnel-Coupled Quantum Dot

We present a technique for manipulating the nuclear spins and the emission polarization from a single optically active quantum dot. When the quantum dot is tunnel coupled to a Fermi sea, we have discovered a natural cycle in which an electron spin is repeatedly created with resonant optical excitation. The spontaneous emission polarization and the nuclear spin polarization exhibit a bistability. For a sigma(+) pump, the emission switches from sigma(+) to sigma(-) at a particular detuning of the laser. Simultaneously, the nuclear spin polarization switches from positive to negative. Away from the bistability, the nuclear spin polarization can be changed continuously from negative to positive, allowing precise control via the laser wavelength.

cond-mat.mes-hall↗

arXiv2010

Radiative cascade from quantum dot metastable spin-blockaded biexciton

We detect a novel radiative cascade from a neutral semiconductor quantum dot. The cascade initiates from a metastable biexciton state in which the holes form a spin-triplet configuration, Pauli-blockaded from relaxation to the spin-singlet ground state. The triplet biexciton has two photon-phonon-photon decay paths. Unlike in the singlet-ground state biexciton radiative cascade, in which the two photons are co-linearly polarized, in the triplet biexciton cascade they are crosslinearly polarized. We measured the two-photon polarization density matrix and show that the phonon emitted when the intermediate exciton relaxes from excited to ground state, preserves the exciton's spin. The phonon, thus, does not carry with it any which-path information other than its energy. Nevertheless, entanglement distillation by spectral filtering was found to be rather ineffective for this cascade. This deficiency results from the opposite sign of the anisotropic electron-hole exchange interaction in the excited exciton relative to that in the ground exciton.

cond-mat.mes-hall↗

arXiv2009

Radiative cascades in charged quantum dots

We measured, for the first time, two photon radiative cascades due to sequential recombination of quantum dot confined electron hole pairs in the presence of an additional spectator charge carrier. We identified direct, all optical cascades involving spin blockaded intermediate states, and indirect cascades, in which non radiative relaxation precedes the second recombination. Our measurements provide also spin dephasing rates of confined carriers.

cond-mat.mes-hall↗

arXiv2008

Dressed excitonic states and quantum interference in a three-level quantum dot ladder system

We observe dressed states and quantum interference effects in a strongly driven three-level quantum dot ladder system. The effect of a strong coupling field on one dipole transition is measured by a weak probe field on the second dipole transition using differential reflection. When the coupling energy is much larger than both the homoge-neous and inhomogeneous linewidths an Autler-Townes splitting is observed. Striking differences are observed when the transitions resonant with the strong and weak fields are swapped, particularly when the coupling energy is nearly equal to the measured linewidth. This result is attributed to quantum interference: a modest destructive or constructive interference is observed depending on the pump / probe geometry. The data demonstrate that coher-ence of both the bi-exciton and the exciton is maintained in this solid-state system, even under intense illumina-tion, which is crucial for prospects in quantum information processing and non-linear optical devices.

cond-mat.mtrl-sci↗

arXiv2008

Coulomb interactions in single, charged self-assembled quantum dots: radiative lifetime and recombination energy

We present results on the charge dependence of the radiative recombination lifetime, Tau, and the emission energy of excitons confined to single self-assembled InGaAs quantum dots. There are significant dot-to-dot fluctuations in the lifetimes for a particular emission energy. To reach general conclusions, we present the statistical behavior by analyzing data recorded on a large number of individual quantum dots. Exciton charge is controlled with extremely high fidelity through an n-type field effect structure, providing access to the neutral exciton (X0), the biexciton (2X0) and the positively (X1+) and negatively (X1-) charged excitons. We find significant differences in the recombination lifetime of each exciton such that, on average, Tau(X1-) / Tau(X0) = 1.25, Tau(X1+) / Tau(X0) = 1.58 and Tau(2X0) / Tau(X0) = 0.65. We attribute the change in lifetime to significant changes in the single particle hole wave function on charging the dot, an effect more pronounced on charging X0 with a single hole than with a single electron. We verify this interpretation by recasting the experimental data on exciton energies in terms of Coulomb energies. We show directly that the electron-hole Coulomb energy is charge dependent, reducing in value by 5-10% in the presence of an additional electron, and that the electron-electron and hole-hole Coulomb energies are almost equal.

cond-mat.mtrl-sci↗

arXiv2007

Polarization sensitive spectroscopy of charged Quantum Dots

We present an experimental and theoretical study of the polarized photoluminescence spectrum of single semiconductor quantum dots in various charge states. We compare our high resolution polarization sensitive spectral measurements with a new many-carrier theoretical model, which was developed for this purpose. The model considers both the isotropic and anisotropic exchange interactions between all participating electron-hole pairs. With this addition, we calculate both the energies and polarizations of all optical transitions between collective, quantum dot confined charge carrier states. We succeed in identifying most of the measured spectral lines. In particular, the lines resulting from singly-, doubly- and triply- negatively charged excitons and biexcitons. We demonstrate that lines emanating from evenly charged states are linearly polarized. Their polarization direction does not necessarily coincide with the traditional crystallographic direction. It depends on the shells of the single carriers, which participate in the recombination process.

cond-mat.mes-hall↗

arXiv2007

Contrast in transmission spectroscopy of a single quantum dot

We perform transmission spectroscopy on single quantum dots and examine the effects of a resident carriers spin, the incident laser spot size, polarization, and power on the experimental contrast. We demonstrate a factor of 4 improvement in the maximum contrast by using a solid immersion lens to decrease the spot area. This increase yields a maximum signal to noise ratio of 2000 Hz-1/2, which will allow for MHz detection frequencies. We anticipate that this improvement will allow further investigation of spectral fluctuation and open up the feasibility for an all-optical read-out of an electron spin in a quantum dot.

cond-mat.mes-hall↗