High resolution coherent population trapping on a single hole spin in a semiconductor
Julien Houel, Jonathan H. Prechtel, Daniel Brunner, Christopher E. Kuklewicz, Brian D. Gerardot, Nick G. Stoltz, Pierre M. Petroff, Richard J. Warburton
We report high resolution coherent population trapping on a single hole spin in a semiconductor quantum dot. The absorption dip signifying the formation of a dark state exhibits an atomic physics-like dip width of just 10 MHz. We observe fluctuations in the absolute frequency of the absorption dip, evidence of very slow spin dephasing. We identify this process as charge noise by, first, demonstrating that the hole spin g-factor in this configuration (in-plane magnetic field) is strongly dependent on the vertical electric field, and second, by characterizing the charge noise through its effects on the optical transition frequency. An important conclusion is that charge noise is an important hole spin dephasing process.
In high-purity n-type GaAs under strong magnetic field, we are able to isolate a lambda system composed of two Zeeman states of neutral-donor bound electrons and the lowest Zeeman state of bound excitons. When the two-photon detuning of this system is zero, we observe a pronounced dip in the excited-state photoluminescence indicating the creation of the coherent population-trapped state. Our data are consistent with a steady-state three-level density-matrix model. The observation of coherent population trapping in GaAs indicates that this and similar semiconductor systems could be used for var…
The role of image charges in nanoporous semiconductor materials is investigated within the framework of the effective mass and envelope function approximations. We show that nanometric air bubbles in these materials can act as electron-trapping centers. This trapping capability originates from a deep stabilizing self-polarization potential well induced by the air - semiconductor dielectric mismatch which can surpass the electroaffinity barrier. The trapping strength is a function of the pore size and the bulk parameters of the matrix material. A {\it trapping parameter} characteristic for each…
We propose a new transport mechanism through tunnel-coupled quantum dots based on the coherent population trapping effect. Coupling to an excited level by the coherent radiation of two microwaves can lead to an extremely narrow current antiresonance. The effect can be used to determine interdot dephasing rates and is a mechanism for a very sensitive, optically controlled current switch.
We consider a three-node fully connected network (Delta network) showing that a coherent population trapping phenomenon occurs, generalizing results for the Lambda network known to support a dark state. Transport in such structures provides signatures of detrapping, which can be triggered by external controls. In the presence of an environment it turns out to be sensitive to its Markovianity. Adiabatic modulation of the system's parameters may yield coherent population transfer, analogous to the stimulated Raman adiabatic passage phenomenon. Robustness of this protocol against non-adiabatic tr…
We propose and theoretically analyze the use of coherent population trapping of a single diamond nitrogen vacancy (NV) center for continuous real-time sensing. The formation of the dark state in coherent population trapping prevents optical emissions from the NV center. Fluctuating magnetic fields, however, can kick the NV center out of the dark state, leading to a sequence of single-photon emissions. A time series of the photon counts detected can be used for magnetic field estimations, even when the average photon count per update time interval is much smaller than 1. For a theoretical demon…
Interlayer excitons (IXs) in 2D semiconductors have long lifetimes and spin-valley coupled physics, with a long-standing goal of single exciton trapping for valleytronic applications. In this work, we use a nano-patterned graphene gate to create an electrostatic IX trap. We measure a unique power-dependent blue-shift of IX energy, where narrow linewidth emission exhibits discrete energy jumps. We attribute these jumps to quantized increases of the number occupancy of IXs within the trap and compare to a theoretical model to assign the lowest energy emission line to single IX recombination.
Optical spin rotations and cycling transitions for measurement are normally incompatible in quantum dots, presenting a fundamental problem for quantum information applications. Here we show that for a hole spin this problem can be addressed using a trion with one hole in an excited orbital, where strong spin-orbit interaction tilts the spin. Then, a particular trion triplet forms a double $Λ$ system, even in a Faraday magnetic field, which we use to demonstrate fast hole spin initialization and coherent population trapping. The lowest trion transitions still strongly preserve spin, thus combin…
Understanding the maximal enhancement of solar absorption in semiconductor materials by light trapping promises the development of affordable solar cells. However, the conventional Lambertian limit is only valid for idealized material systems with weak absorption, and cannot hold for the typical semiconductor materials used in solar cells due to the substantial absorption of these materials. Herein we theoretically demonstrate the maximal solar absorption enhancement for semiconductor materials and elucidate the general design principle for light trapping structures to approach the theoretical…
Hybrid spin-optomechanical quantum systems offer high flexibility, integrability and applicability for quantum science and technology. Particularly, on-chip surface acoustic waves (SAWs) can efficiently drive spin transitions in the ground states (GSs) of atomic-scale, color centre qubits, which are forbidden in case of the more frequently used electromagnetic fields. Here, we demonstrate that strain-induced spin interactions within their optically excited state (ES) can exceed by two orders of magnitude the ones within the GS. This gives rise to novel physical phenomena, such as the acoustica…
We experimentally demonstrate how coherent population trapping (CPT) for donor-bound electron spins in GaAs results in autonomous feedback that prepares stabilized states for the spin polarization of nuclei around the electrons. CPT was realized by excitation with two lasers to a bound-exciton state. Transmission studies of the spectral CPT feature on an ensemble of electrons directly reveal the statistical distribution of prepared nuclear spin states. Tuning the laser driving from blue to red detuned drives a transition from one to two stable states. Our results have importance for ongoing re…
Quantum interference is a natural consequence of wave-particle duality in quantum mechanics, and is widely observed at the atomic scale. One interesting manifestation of quantum interference is coherent population trapping (CPT), first proposed in three-level driven atomic systems and observed in quantum optical experiments. Here, we demonstrate CPT in a gate-defined semiconductor double quantum dot (DQD), with some unique twists as compared to the atomic systems. Specifically, we observe CPT in both driven and non-driven situations. We further show that CPT in a driven DQD could be used to ge…
Coherent population trapping at zero magnetic field was observed for nitrogen-vacancy centers in diamond under optical excitation. This was measured as a reduction in photoluminescence when the detuning between two excitation lasers matched the 2.88 GHz crystal-field splitting of the color center ground states. This behavior is highly sensitive to strain, which modifies the excited states, and was unexpected following recent experiments demonstrating optical readout of single nitrogen-vacancy electron spins based on cycling transitions. These results demonstrate for the first time that three-l…
For quantum technologies based on single excitons and spins, the deterministic placement and control of a single exciton is a long-standing goal. MoSe2-WSe2 heterostructures host spatially indirect interlayer excitons (IXs) which exhibit highly tunable energies and unique spin-valley physics, making them promising candidates for quantum information processing. Previous IX trapping approaches involving moiré superlattices and nanopillars do not meet the quantum technology requirements of deterministic placement and energy tunability. Here, we use a nanopatterned graphene gate to create a sharpl…
Hyperfine interactions with a nuclear spin environment fundamentally limit the coherence properties of confined electron spins in the solid-state. Here, we show that a quantum interference effect in optical absorption from two electronic spin states of a solid-state emitter can be used to prepare the surrounding environment of nuclear spins in well-defined states, thereby suppressing electronic spin dephasing. The evolution of the coupled electron-nuclei system into a coherent population trapping state by optical excitation induced nuclear spin diffusion can be described in terms of Levy fligh…
Coherent population trapping (CPT) refers to the steady-state trapping of population in a coherent superposition of two ground states which are coupled by coherent optical fields to an intermediate state in a three-level atomic system. Recently, CPT has been observed in an ensemble of donor bound spins in GaAs and in single nitrogen vacancy centers in diamond by using a fluorescence technique. Here we report the demonstration of CPT of an electron spin in a single quantum dot (QD) charged with one electron.
Coherent population trapping (CPT) provides a highly sensitive means for probing the energy level structure of an atomic system. For a nitrogen vacancy center in diamond, the CPT offers an alternative to the standard optically-detected magnetic resonance method for measuring the hyperfine structure of the electronic ground states. We show that the nuclear spin dependent CPT measures directly the hyperfine splitting of these states due to the 14N nuclear spin. The CPT spectral response obtained in the presence of a strong microwave field, resonant or nearly resonant with a ground state spin tra…
We predict that conduction electrons in a semiconductor film containing a centered square array of metal nanowires normal to its plane are bound in quantum states around the central wires, if a positive bias voltage is applied between the wires at the square vertices and these latter. We obtain and discuss the eigenenergies and eigenfunctions of two models with different dimensions. The results show that the eigenstates can be grouped into different shells. The energy differences between the shells is typically a few tens of meV, which corresponds to frequencies of emitted or absorbed photons …
We propose a solid-state implementation of stimulated Raman adiabatic passage in two coupled semiconductor quantum dots. Proper combination of two pulsed laser fields allows the coherent carrier transfer between the two nanostructures without suffering significant losses due to environment coupling. By use of a general solution scheme for the carrier states in the double-dot structure, we identify the pertinent dot and laser parameters.
Nonradiative processes limit optoelectronic functionality of nanocrystals and curb their device performance. Nevertheless, the dynamic structural origins of nonradiative relaxations in nanocrystals are not understood. Here, femtosecond electron diffraction measurements corroborated by atomistic simulations uncover transient lattice deformations accompanying radiationless electronic processes in semiconductor nanocrystals. Investigation of the excitation energy dependence shows that hot carriers created by a photon energy considerably larger than the bandgap induce structural distortions at nan…
Divacancy defects in silicon carbide have long-lived electronic spin states and sharp optical transitions, with properties that are similar to the nitrogen-vacancy defect in diamond. We report experiments on 4H-SiC that investigate all-optical addressing of spin states with the zero-phonon-line transitions. Our magneto-spectroscopy results identify the spin $S=1$ structure of the ground and excited state, and a role for decay via intersystem crossing. We use these results for demonstrating coherent population trapping of spin states with divacancy ensembles that have particular orientations in…
Atomically-thin transition metal dichalcogenide crystals (TMDCs) hold great promise for future semiconductor optoelectronics due to their unique electronic and optical properties. In particular, electron-hole pairs (excitons) in TMDCs are stable at room temperature and interact strongly with light. When TMDCs are embedded in an optical microcavity, the excitons can hybridise with cavity photons to form exciton polaritons (polaritons herein), which display both ultrafast velocities and strong interactions. The ability to manipulate and trap polaritons on a microchip is critical for future appli…
We present a fully electronic analogue of coherent population trapping in quantum optics, based on destructive interference of single-electron tunneling between three quantum dots. A large bias voltage plays the role of the laser illumination. The trapped state is a coherent superposition of the electronic charge in two of these quantum dots, so it is destabilized as a result of decoherence by coupling to external charges. The resulting current I through the device depends on the ratio of the decoherence rate Gamma_phi and the tunneling rates. For Gamma_phi --> 0 one has simply I=e Gamma_phi. …
A robust scheme for state preparation and state trapping for the spins of two electrons in a semiconductor double quantum dot is presented. The system is modeled by two spins coupled to two independent bosonic reservoirs. Decoherence effects due to this environment are minimized by application of optimized control fields which make the target state to the ground state of the isolated driven spin system. We show that stable spin entanglement with respect to pure dephasing is possible. Specifically, we demonstrate state trapping in a maximally entangled state (Bell state) in the presence of deco…
Destructive interference of single-electron tunneling between three quantum dots can trap an electron in a coherent superposition of charge on two of the dots. Coupling to external charges causes decoherence of this superposition, and in the presence of a large bias voltage each decoherence event transfers a certain number of electrons through the device. We calculate the counting statistics of the transferred charges, finding a crossover from sub-Poissonian to super-Poissonian statistics with increasing ratio of tunnel and decoherence rates.
Designing coherent processes is essential for developing quantum information technologies. We study coherent dynamics of two spatially separated electrons in a coupled semiconductor double quantum dot (DQD), in which various two-qubit operations are demonstrated just by adjusting the gate voltages. Especially, second-order correlated coherent oscillations provide functional quantum processes for making quantum correlation of separated particles. The results encourage searching quantum entanglement in electronic devices.
We study the localization of dressed Dirac electrons in a cylindrical quantum dot (QD) formed on monolayer and bilayer graphene by spatially different potential profiles. Short lived excitonic states which are too broad to be resolved in linear spectroscopy are revealed by cross peaks in the photon-echo nonlinear technique. Signatures of the dynamic gap in the two-dimensional spectra are discussed. The effect of the Coulomb induced exciton-exciton scattering and the formation of biexciton molecules are demonstrated.
Bandgap control is of central importance for semiconductor technologies. The traditional means of control is to dope the lattice chemically, electrically or optically with charge carriers. Here, we demonstrate for the first time a widely tunable bandgap (renormalisation up to 650 meV at room-temperature) in two-dimensional (2D) semiconductors by coherently doping the lattice with plasmonic hot electrons. In particular, we integrate tungsten-disulfide (WS$_2$) monolayers into a self-assembled plasmonic crystal, which enables coherent coupling between semiconductor excitons and plasmon resonance…
We investigate the coherent dynamics of carriers in semiconductor superlattices driven by ac-dc electric fields. We solve numerically the time-dependent effective-mass equation for the envelope function. We find that carriers undergo Rabi oscillations when the driving frequency is close to the separation between minibands.
new defect-assisted mechanism of multiphonon intraband carrier relaxation in semiconductor quantum dots, where the carrier is found in a coherent superposition of the initial, final, and defect states, is proposed. It is shown that this mechanism is capable of explaining the observed trends in temperature dependences of the intraband relaxation rates for PbSe and CdSe colloidal nanocrystal quantum dots.
As basic elements of the quantum computer - quantum bits (qubits) we offer semiconductor quantum dots containing one electron each and consisting each of two tunnel-connected parts. The numerical solution of a Schroedinger equation with the account of Coulomb field of adjacent electrons shows, that in such structures the realization of a full set of basic logic operations which are necessary for fulfillment of quantum computations is possible. Durations of one- and two-qubit operations versus qubit geometry are obtained. Decoherence rates due to spontaneous emission of phonons and acoustic pho…
We propose a new approach to coherent control of transport via molecular junctions, which bypasses several of the hurdles to experimental realization of optically manipulated nanoelectronics noted in the previous literature. The method is based on the ap-plication of intrinsic semiconductor contacts and optical frequencies below the semiconductor bandgap. It relies on a simple and general concept, namely the controllable photonic replication of molecular levels through the dipole driving the molecular bridge by an electromagnetic field. We predict the effect of coherent destruction of induced …
Two-dimensional (2D) magnetic semiconductors feature both tightly-bound excitons with large oscillator strength and potentially long-lived coherent magnons due to the presence of bandgap and spatial confinement. While magnons and excitons are energetically mismatched by orders of magnitude, their coupling can lead to efficient optical access to spin information. Here we report strong magnon-exciton coupling in the 2D van der Waals (vdW) antiferromagnetic (AFM) semiconductor CrSBr. Coherent magnons launched by above-gap excitation modulate the interlayer hybridization, which leads to dynamic mo…
We review the topic of Bose-Einstein condensation of excitons in semiconductors, focusing on the signatures of the macroscopic order of the exciton condensate.
We review some experimental and theoretical aspects of coherent acoustic phonon generation in piezoelectric semiconductor multiple quantum wells. In order to model more advanced and complicated nano-acoustic devices, a macroscopic continuum theory for the generation and propagation of coherent acoustic phonons in piezoelectric semiconductor heterostructures is presented. The macroscopic approach is applicable in the coherent regime, and can be easily utilized to study coherent acoustic devices based on piezoelectric semiconductor heterosutructures. For each phonon mode, the corresponding coher…
In condensed-matter physics, remarkable advances have been made with atomic systems by establishing a thorough control over cooling and trapping techniques. In semiconductors, this method may also provide a deterministic approach to reach the long standing goal of harnessing collective quantum phenomena with exciton gases. While long-lived excitons are simply cooled to very low temperatures using cryogenic apparatus, engineering confining potentials has been a challenging task. This degree of control was only achieved recently with devices realized by highly demanding nano-fabrication processe…
We use the spin-polarized excitons in a single quantum dot to design optical controls for basic operations in quantum computing. We examine the ultrafast nonlinear optical processes required and use the coherent nonlinear optical responses to deduce if such processes are physically reasonable. The importance and construction of an entangled state of polarized exciton states in a single quantum dot is explained. We put our proposal in perspective with respect to a number of theoretical suggestions of utilizing the semiconductor quantum dots.
The coherent spin dynamics of resident carriers, electrons and holes, in semiconductor quantum structures is studied by periodical optical excitation using short laser pulses and in an external magnetic field. The generation and dephasing of spin polarization in an ensemble of carrier spins, for which the relaxation time of individual spins exceeds the repetition period of the laser pulses, are analyzed theoretically. Spin polarization accumulation is manifested either as resonant spin amplification or as mode-locking of carrier spin coherences. It is shown that both regimes have the same orig…
Excitonic contributions to absorption and photocurrent generation in semiconductor nanostructures are described theoretically and simulated numerically using steady-state non-equilibrium Green's function theory. In a first approach, the coherent interband polarization including Coulomb corrections is determined from a Bethe-Salpeter-type equation for the equal time interband single-particle charge carrier Green's function. The effects of excitonic absorption on photocurrent generation are considered on the same level of approximation via the derivation of the corresponding corrections to the e…
Multidimensional coherent spectroscopy (MDCS) is used to separate coherent and incoherent many-body contributions to the population-time dynamics in a GaAs-based semiconductor microcavity encapsulating a single InGaAs quantum well. In a three-pulse four-wave-mixing scheme, the second delay time is the population time that in MDCS probes excited-state coherences and population dynamics. Nonlinear optical interactions can mix these contributions, which are isolated here for the lower- and upper-exciton-polariton through the self- and mutual-interaction features. Results show fast decays and osci…
We performed low temperature shot noise measurements in Superconductor (TiN) - strongly disordered normal metal (heavily doped Si) weakly transparent junctions. We show that the conductance has a maximum due to coherent multiple reflections at low energy and that shot noise is then twice the Poisson noise (S=4eI). The shot noise changes to the normal value (S=2eI) due to a large quasiparticle contribution.