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A. I. Tartakovskii

Publications and source records attributed to A. I. Tartakovskii.

At least 37 records · Page 2Linked to original sources

Few-second-long correlation times in a quantum dot nuclear spin bath probed by frequency-comb NMR spectroscopy

One of the key challenges in spectroscopy is inhomogeneous broadening that masks the homogeneous spectral lineshape and the underlying coherent dynamics. A variety of techniques including four-wave mixing and spectral hole-burning are used in optical spectroscopy while in nuclear magnetic resonance (NMR) spin-echo is the most common way to counteract inhomogeneity. However, the high-power pulses used in spin-echo and other sequences often create spurious dynamics obscuring the subtle spin correlations that play a crucial role in quantum information applications. Here we develop NMR techniques that allow the correlation times of the fluctuations in a nuclear spin bath of individual quantum dots to be probed. This is achieved with the use of frequency comb excitation which allows the homogeneous NMR lineshapes to be measured avoiding high-power pulses. We find nuclear spin correlation times exceeding 1 s in self-assembled InGaAs quantum dots - four orders of magnitude longer than in strain-free III-V semiconductors. The observed freezing of the nuclear spin fluctuations opens the way for the design of quantum dot spin qubits with a well-understood, highly stable nuclear spin bath.

cond-mat.mes-hall↗

Exciton-polaritons in van der Waals heterostructures embedded in tunable microcavities

Layered materials can be assembled vertically to fabricate a new class of van der Waals (VDW) heterostructures a few atomic layers thick, compatible with a wide range of substrates and optoelectronic device geometries, enabling new strategies for control of light-matter coupling. Here, we incorporate molybdenum diselenide/boron nitride (MoSe$_2$/hBN) quantum wells (QWs) in a tunable optical microcavity. Part-light-part-matter polariton eigenstates are observed as a result of the strong coupling between MoSe$_2$ excitons and cavity photons, evidenced from a clear anticrossing between the neutral exciton and the cavity modes with a splitting of 20 meV for a single MoSe$_2$ monolayer QW, enhanced to 29 meV in MoSe$_2$/hBN/MoSe$_2$ double-QWs. The splitting at resonance provides an estimate of the exciton radiative lifetime of 0.4 ps. Our results pave the way for room temperature polaritonic devices based on multiple-QW VDW heterostructures, where polariton condensation and electrical polariton injection through the incorporation of graphene contacts may be realised.

cond-mat.mes-hall↗

Optical properties of two-dimensional gallium chalcogenide films

Gallium chalcogenides are promising building blocks for novel van der Waals heterostructures. We report low-temperature micro-photoluminescence (PL) of GaTe and GaSe films with thickness ranging from from 200 nm to a single unit cell. In both materials, PL shows dramatic decrease by 10$^4$-10$^5$ when film thickness is reduced from 200 to 10 nm. Based on evidence from cw and time-resolved PL, we propose a model explaining the PL decrease as a result of non-radiative carrier escape via surface states.

cond-mat.mes-hall↗

Light-emitting diodes by bandstructure engineering in van der Waals heterostructures

The advent of graphene and related 2D materials has recently led to a new technology: heterostructures based on these atomically thin crystals. The paradigm proved itself extremely versatile and led to rapid demonstration of tunnelling diodes with negative differential resistance, tunnelling transistors5, photovoltaic devices, etc. Here we take the complexity and functionality of such van der Waals heterostructures to the next level by introducing quantum wells (QWs) engineered with one atomic plane precision. We describe light emitting diodes (LEDs) made by stacking up metallic graphene, insulating hexagonal boron nitride (hBN) and various semiconducting monolayers into complex but carefully designed sequences. Our first devices already exhibit extrinsic quantum efficiency of nearly 10% and the emission can be tuned over a wide range of frequencies by appropriately choosing and combining 2D semiconductors (monolayers of transition metal dichalcogenides). By preparing the heterostructures on elastic and transparent substrates, we show that they can also provide the basis for flexible and semi-transparent electronics. The range of functionalities for the demonstrated heterostructures is expected to grow further with increasing the number of available 2D crystals and improving their electronic quality.

cond-mat.mes-hall↗

Nuclear magnetic resonance inverse spectra of InGaAs quantum dots: Atomistic level structural information

A wealth of atomistic information is contained within a self-assembled quantum dot (QD), associated with its chemical composition and the growth history. In the presence of quadrupolar nuclei, as in InGaAs QDs, much of this is inherited to nuclear spins via the coupling between the strain within the polar lattice and the electric quadrupole moments of the nuclei. Here, we present a computational study of the recently introduced inverse spectra nuclear magnetic resonance technique to assess its suitability for extracting such structural information. We observe marked spectral differences between the compound InAs and alloy InGaAs QDs. These are linked to the local biaxial and shear strains, and the local bonding configurations. The cation-alloying plays a crucial role especially for the arsenic nuclei. The isotopic line profiles also largely differ among nuclear species: While the central transition of the gallium isotopes have a narrow linewidth, those of arsenic and indium are much broader and oppositely skewed with respect to each other. The statistical distributions of electric field gradient (EFG) parameters of the nuclei within the QD are analyzed. The consequences of various EFG axial orientation characteristics are discussed. Finally, the possibility of suppressing the first-order quadrupolar shifts is demonstrated by simply tilting the sample with respect to the static magnetic field.

cond-mat.mes-hall↗

Two-dimensional metal-chalcogenide films in tunable optical microcavities

Quasi-two-dimensional (2D) films of layered metal-chalcogenides have attractive optoelectronic properties. However, photonic applications of thin films may be limited owing to weak light absorption and surface effects leading to reduced quantum yield. Integration of 2D films in optical microcavities will permit these limitations to be overcome owing to modified light coupling with the films. Here we present tunable microcavities with embedded monolayer MoS2 or few monolayer GaSe films. We observe significant modification of spectral and temporal properties of photoluminescence (PL): PL is emitted in spectrally narrow and wavelength-tunable cavity modes with quality factors up to 7400; PL life-time shortening by a factor of 10 is achieved, a consequence of Purcell enhancement of the spontaneous emission rate. This work has potential to pave the way to microcavity-enhanced light-emitting devices based on layered 2D materials and their heterostructures, and also opens possibilities for cavity QED in a new material system of van der Waals crystals.

cond-mat.mtrl-sci↗

Quadrupolar induced suppression of nuclear spin bath fluctuations in self-assembled quantum dots

Decoherence in quantum logic gates (qubits) due to interaction with the surrounding environment is a major obstacle to the practical realization of quantum information technologies. For solid state electron-spin qubits the interaction with nuclear spins is the main problem. One particular, neradicable source of electron decoherence arises from decoherence of the nuclear spin bath, driven by nuclear-nuclear dipolar interactions. Due to its many-body nature nuclear decoherence is difficult to predict, especially for an important class of strained nanostructures where nuclear quadrupolar effects have a significant but largely unknown impact. Here we report direct measurement of nuclear spin bath coherence in individual strained InGaAs/GaAs quantum dots: nuclear spin-echo coherence times in the range T2~1.2 - 4.5 ms are found. Based on these T2 values we demonstrate that quadrupolar interactions make nuclear fluctuations in strained quantum dots much slower compared to lattice matched GaAs/AlGaAs structures. Such fluctuation suppression is particularly strong for arsenic nuclei due to the effect of atomic disorder of gallium and indium alloying. Our findings demonstrate that quadrupolar effects can help to solve the long-standing challenge of designing a scalable hardware for quantum computation: III-V semiconductor spin-qubits can be engineered to have a noise-free nuclear spin bath (previously achievable only in nuclear spin-0 semiconductors, where qubit network interconnection and scaling is challenging).

cond-mat.mes-hall↗

Optical investigation of the natural electron doping in thin MoS2 films deposited on dielectric substrates

Two-dimensional (2D) compounds provide unique building blocks for novel layered devices and hybrid photonic structures. However, large surface-to-volume ratio in thin films enhances the significance of surface interactions and charging effects requiring new understanding. Here we use micro-photoluminescence (PL) and ultrasonic force microscopy to explore the influence of the dielectric environment on optical properties of a few monolayer MoS2 films. PL spectra for MoS2 films deposited on SiO2 substrates are found to vary widely. This film-to-film variation is suppressed by additional capping of MoS2 with SiO2 and SiN, improving mechanical coupling of MoS2 with surrounding dielectrics. We show that the observed PL non-uniformities are related to strong variation in the local electron charging of MoS2 films. In completely encapsulated films, negative charging is enhanced leading to uniform optical properties. Observed great sensitivity of optical characteristics of 2D films to surface interactions has important implications for optoelectronics applications of layered materials.

cond-mat.mtrl-sci↗

The dynamics of amplified spontaneous emission in CdSe/ZnSe quantum dots

We have used the variable stripe technique and pump-probe spectroscopy to investigate both gain and the dynamics of amplified spontaneous emission from CdSe quantum dot structures. We have found modal gain coefficients of 75 and 32 1/cm for asymmetric and symmetric waveguide structures, respectively. Amplified spontaneous emission decay times of 150 and 300 ps and carrier capture times of 15 and 40 ps were measured for the structures with high and low material gains respectively. The difference in the capture times are related to the fact that for the symmetric waveguide, carriers diffuse into the active region from the uppermost ZnMgSSe cladding layer, yielding a longer rise time for the pump-probe signals for this sample.

cond-mat.mtrl-sci↗

Dynamic nuclear polarization in InGaAs/GaAs and GaAs/AlGaAs quantum dots under non-resonant ultra-low power optical excitation

We study experimentally the dependence of dynamic nuclear spin polarization on the power of non-resonant optical excitation in two types of individual neutral semiconductor quantum dots: InGaAs/GaAs and GaAs/AlGaAs. We show that the mechanism of nuclear spin pumping via second order recombination of optically forbidden (''dark'') exciton states recently reported in InP/GaInP quantum dots [Phys. Rev. B 83, 125318 (2011)] is relevant for material systems considered in this work. In the InGaAs/GaAs dots this nuclear spin polarization mechanism is particularly pronounced, resulting in Overhauser shifts up to ~80 micro-eV achieved at optical excitation power ~1000 times smaller than the power required to saturate ground state excitons. The Overhauser shifts observed at low-power optical pumping in the interface GaAs/AlGaAs dots are generally found to be smaller (up to ~40 micro-eV). Furthermore in GaAs/AlGaAs we observe dot-to-dot variation and even sign reversal of the Overhauser shift which is attributed to dark-bright exciton mixing originating from electron-hole exchange interaction in dots with reduced symmetry. Nuclear spin polarization degrees reported in this work under ultra-low power optical pumping are comparable to those achieved by techniques such as resonant optical pumping or above-gap pumping with high power circularly polarized light. Dynamic nuclear polarization via second-order recombination of ''dark'' excitons may become a useful tool in single quantum dot applications, where manipulation of the nuclear spin environment or electron spin is required.

cond-mat.mes-hall↗

Isotope sensitive measurement of the hole-nuclear spin interaction in quantum dots

Decoherence caused by nuclear field fluctuations is a fundamental obstacle to the realization of quantum information processing using single electron spins. Alternative proposals have been made to use spin qubits based on valence band holes having weaker hyperfine coupling. However, it was demonstrated recently both theoretically and experimentally that the hole hyperfine interaction is not negligible, although a consistent picture of the mechanism controlling the magnitude of the hole-nuclear coupling is still lacking. Here we address this problem by performing isotope selective measurement of the valence band hyperfine coupling in InGaAs/GaAs, InP/GaInP and GaAs/AlGaAs quantum dots. Contrary to existing models we find that the hole hyperfine constant along the growth direction of the structure (normalized by the electron hyperfine constant) has opposite signs for different isotopes and ranges from -15% to +15%. We attribute such changes in hole hyperfine constants to the competing positive contributions of p-symmetry atomic orbitals and the negative contributions of d-orbitals. Furthermore, we find that the d-symmetry contribution leads to a new mechanism for hole-nuclear spin flips which may play an important role in hole spin decoherence. In addition the measured hyperfine constants enable a fundamentally new approach for verification of the computed Bloch wavefunctions in the vicinity of nuclei in semiconductor nanostructures.

cond-mat.mes-hall↗

Effect of the GaAsP shell on optical properties of self-catalyzed GaAs nanowires grown on silicon

We realize growth of self-catalyzed core-shell GaAs/GaAsP nanowires (NWs) on Si substrates using molecular-beam epitaxy. Transmission electron microscopy (TEM) of single GaAs/GaAsP NWs confirms their high crystal quality and shows domination of the zinc-blende phase. This is further confirmed in optics of single NWs, studied using cw and time-resolved photoluminescence (PL). A detailed comparison with uncapped GaAs NWs emphasizes the effect of the GaAsP capping in suppressing the non-radiative surface states: significant PL enhancement in the core-shell structures exceeding 2000 times at 10K is observed; in uncapped NWs PL is quenched at 60K whereas single core-shell GaAs/GaAsP NWs exhibit bright emission even at room temperature. From analysis of the PL temperature dependence in both types of NW we are able to determine the main carrier escape mechanisms leading to the PL quench.

cond-mat.mtrl-sci↗

High resolution nuclear magnetic resonance spectroscopy of highly-strained quantum dot nanostructures

Much new solid state technology for single-photon sources, detectors, photovoltaics and quantum computation relies on the fabrication of strained semiconductor nanostructures. Successful development of these devices depends strongly on techniques allowing structural analysis on the nanometer scale. However, commonly used microscopy methods are destructive, leading to the loss of the important link between the obtained structural information and the electronic and optical properties of the device. Alternative non-invasive techniques such as optically detected nuclear magnetic resonance (ODNMR) so far proved difficult in semiconductor nano-structures due to significant strain-induced quadrupole broadening of the NMR spectra. Here, we develop new high sensitivity techniques that move ODNMR to a new regime, allowing high resolution spectroscopy of as few as 100000 quadrupole nuclear spins. By applying these techniques to individual strained self-assembled quantum dots, we measure strain distribution and chemical composition in the volume occupied by the confined electron. Furthermore, strain-induced spectral broadening is found to lead to suppression of nuclear spin magnetization fluctuations thus extending spin coherence times. The new ODNMR methods have potential to be applied for non-invasive investigations of a wide range of materials beyond single nano-structures, as well as address the task of understanding and control of nuclear spins on the nanoscale, one of the central problems in quantum information processing.

cond-mat.mes-hall↗

Charge control in InP/GaInP single quantum dots embedded in Schottky diodes

We demonstrate control by applied electric field of the charge states in single self-assembled InP quantum dots placed in GaInP Schottky structures grown by metalorganic vapor phase epitaxy. This has been enabled by growth optimization leading to suppression of formation of large dots uncontrollably accumulating charge. Using bias- and polarization-dependent micro-photoluminescence, we identify the exciton multi-particle states and carry out a systematic study of the neutral exciton state dipole moment and polarizability. This analysis allows for the characterization of the exciton wavefunction properties at the single dot level for this type of quantum dots. Photocurrent measurements allow further characterization of exciton properties by electrical means, opening new possibilities for resonant excitation studies for such system.

cond-mat.mes-hall↗

Full coherent control of nuclear spins in an optically pumped single quantum dot

Highly polarized nuclear spins within a semiconductor quantum dot (QD) induce effective magnetic (Overhauser) fields of up to several Tesla acting on the electron spin or up to a few hundred mT for the hole spin. Recently this has been recognized as a resource for intrinsic control of QD-based spin quantum bits. However, only static long-lived Overhauser fields could be used. Here we demonstrate fast redirection on the microsecond time-scale of Overhauser fields of the order of 0.5 T experienced by a single electron spin in an optically pumped GaAs quantum dot. This has been achieved using full coherent control of an ensemble of 10^3-10^4 optically polarized nuclear spins by sequences of short radio-frequency (rf) pulses. These results open the way to a new class of experiments using rf techniques to achieve highly-correlated nuclear spins in quantum dots, such as adiabatic demagnetization in the rotating frame leading to sub-micro K nuclear spin temperatures, rapid adiabatic passage, and spin squeezing.

cond-mat.mes-hall↗

Direct measurement of the hole-nuclear spin interaction in single quantum dots

We use photoluminescence spectroscopy of ''bright'' and ''dark'' exciton states in single InP/GaInP quantum dots to measure hyperfine interaction of the valence band hole with nuclear spins polarized along the sample growth axis. The ratio of the hyperfine constants for the hole (C) and electron (A) is found to be C/A~-0.11. In InP dots the contribution of spin 1/2 phosphorus nuclei to the hole-nuclear interaction is weak, which enables us to determine experimentally the value of C for spin 9/2 indium nuclei as C_In~-5 micro-eV. This high value of C is in good agreement with recent theoretical predictions and suggests that the hole-nuclear spin interaction has to be taken into account when considering spin qubits based on holes.

cond-mat.mes-hall↗

Alignment of nuclear spins in single quantum dots using unpolarized light

We report optical pumping of neutral quantum dots leading to nuclear spin alignment with direction insensitive to polarization and wavelength of light. Measurements of photoluminescence of both "dark" and "bright" excitons in single dots reveal that nuclear spin pumping occurs via a virtual spin-flip transition between these states accompanied by photon emission. The sign of the nuclear spin polarization is determined by asymmetry in the exciton energy spectrum, rather than by the sign of the exciton spin polarization.

cond-mat.mes-hall↗

Optically tunable nuclear magnetic resonance in a single quantum dot

We report optically detected nuclear magnetic resonance (ODNMR) measurements on small ensembles of nuclear spins in single GaAs quantum dots. Using ODNMR we make direct measurements of the inhomogeneous Knight field from a photo-excited electron which acts on the nuclei in the dot. The resulting shifts of the NMR peak can be optically controlled by varying the electron occupancy and its spin orientation, and lead to strongly asymmetric lineshapes at high optical excitation. The all-optical control of the NMR lineshape will enable position-selective control of small groups of nuclear spins in a dot. Our calculations also show that the asymmetric NMR peak lineshapes can provide information on the volume of the electron wave-function, and may be used for measurements of non-uniform distributions of atoms in nano-structures.

cond-mat.mes-hall↗