arXiv subjects

E. A. Chekhovich

Publications and source records attributed to E. A. Chekhovich.

At least 19 recordsLinked to original sources

arXiv2018

Direct measurement of hyperfine shifts and radiofrequency manipulation of the nuclear spins in individual CdTe/ZnTe quantum dots

We achieve direct detection of electron hyperfine shifts in individual CdTe/ZnTe quantum dots. For the previously inaccessible regime of strong magnetic fields $B_z\gtrsim0.1$ T, we demonstrate robust polarization of a few-hundred-particle nuclear spin bath, with optical initialization time of $\sim$ 1 ms and polarization lifetime exceeding $\sim$ 1 s. Nuclear magnetic resonance spectroscopy of individual dots reveals strong electron-nuclear interactions characterized by the Knight fields $|B_e|\gtrsim50$ mT, an order of magnitude stronger than in III-V semiconductor quantum dots. Our studies confirm II-VI semiconductor quantum dots as a promising platform for hybrid electron-nuclear spin quantum registers, combining the excellent optical properties comparable to III-V dots, and the dilute nuclear spin environment similar to group-IV semiconductors.

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arXiv2018

Cross-calibration of GaAs deformation potentials and gradient-elastic tensors using photoluminescence and nuclear magnetic resonance spectroscopy in GaAs/AlGaAs quantum dot structures

Lattice matched GaAs/AlGaAs epitaxial structures with quantum dots are studied under static uniaxial stress applied either along the $[001]$ or $[110]$ crystal directions. We conduct simultaneous measurements of the spectral shifts in the photoluminescence of the bulk GaAs substrate, which relate to strain via deformation potentials $a$ and $b$, and the quadrupolar shifts in the optically detected nuclear magnetic resonance spectra of the quantum dots, which relate to the same strain via the gradient-elastic tensor $S_{ijkl}$. Measurements in two uniaxial stress configurations are used to derive the ratio $b/a=0.241\pm0.008$ in good agreement with previous studies on GaAs. Based on the previously estimated value of $a\approx-8.8$ eV we derive the product of the nuclear quadrupolar moment $Q$ and the $S$-tensor diagonal component in GaAs to be $QS_{11}\approx+0.76\times10^{-6}$ V for $^{75}$As and $QS_{11}\approx-0.37\times10^{-6}$ V for $^{69}$Ga nuclei. In our experiments the signs of $S_{11}$ are directly measurable, which was not possible in the earlier nuclear acoustic resonance studies. Our $QS_{11}$ values are a factor of $\sim$1.4 smaller than those derived from the nuclear acoustic resonance experiments [Phys. Rev. B 10, 4244 (1974)]. The gradient-elastic tensor values measured in this work can be applied in structural analysis of strained III-V semiconductor nanostructures via accurate modelling of their magnetic resonance spectra.

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arXiv2017

Dynamical suppression of fluctuations in an interacting nuclear spin bath of a self-assembled quantum dot using multiple pulse nuclear magnetic resonance

Electron spin qubit coherence in quantum dots is ultimately limited by random nuclear spin bath fluctuations. Here we aim to eliminate this randomness by making spin bath evolution deterministic. We introduce spin bath control sequences, which systematically combine Hahn and solid echoes to suppress inhomogeneous broadening and nuclear-nuclear interactions. Experiments on self-assembled quantum dots show a five-fold increase in nuclear spin coherence. Numerical simulations show that these sequences can be used to suppress decoherence via qubit-qubit interaction in point defect and dopant spin systems.

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arXiv2017

MOVPE growth, transmission electron microscopy and magneto-optical spectroscopy of individual InAsP/GaInP quantum dots

We report on growth and characterization of individual InAsP/GaInP quantum dots with variable nominal As molar fraction. Magneto-photoluminescence experiments reveal QD emission in a wide range from 1.3 to 1.8 eV confirming incorporation of As into quantum dots. Transmission electron microscopy reveals a core-cap structure of InAsP quantum dots with an InAs-rich core capped by an InP-rich layer. Inside the core, an As molar fraction up to x=0.12 is observed. The heavy hole g-factor is found to be strongly dependent on As molar fraction, while the electron g-factor is close to the InP values. This suggests type-II carrier confinement in the studied InAsP dots with holes (electrons) localized in the core (cap) region. Finally, dynamic nuclear polarization is observed which allows for further insight into structural properties using nuclear magnetic resonance.

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arXiv2017

Measurement of the spin temperature of optically cooled nuclei and GaAs hyperfine constants in GaAs/AlGaAs quantum dots

Deep cooling of electron and nuclear spins is equivalent to achieving polarization degrees close to 100% and is a key requirement in solid state quantum information technologies. While polarization of individual nuclear spins in diamond and SiC reaches 99% and beyond, it has been limited to 60-65% for the nuclei in quantum dots. Theoretical models have attributed this limit to formation of coherent "dark" nuclear spin states but experimental verification is lacking, especially due to the poor accuracy of polarization degree measurements. Here we measure the nuclear polarization in GaAs/AlGaAs quantum dots with high accuracy using a new approach enabled by manipulation of the nuclear spin states with radiofrequency pulses. Polarizations up to 80% are observed - the highest reported so far for optical cooling in quantum dots. This value is still not limited by nuclear coherence effects. Instead we find that optically cooled nuclei are well described within a classical spin temperature framework. Our findings unlock a route for further progress towards quantum dot electron spin qubits where deep cooling of the mesoscopic nuclear spin ensemble is used to achieve long qubit coherence. Moreover, GaAs hyperfine material constants are measured here experimentally for the first time.

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arXiv2015

Photoluminescence and Raman investigation of stability of InSe and GaSe thin films

Layered III-chalcogenide compounds belong to a variety of layered crystals that can be implemented in van der Waals heterostructures. Here we report an optical study of the stability of two of these compounds: indium selenide (InSe) and gallium selenide (GaSe). Micro-photoluminescence (PL) and Raman spectroscopy are used to determine how the properties of thin films of these materials change when they are exposed to air at room temperature. We find that in GaSe films, PL signal decreases on average below 50% over 24 (72) hours of exposure for films with thicknesses 10-25 (48-75) nm. In contrast, weak PL decrease of less than 20% is observed for InSe nm films after exposure of 100 hours. Similar trends are observed in Raman spectroscopy: within a week, the Raman signal decreases by a factor of 10 for a 24 nm thick GaSe, whereas no decrease was found for a 16 nm InSe film. We estimate that when exposed to air, the layers adjacent to the GaSe film surface degrade and become non-luminescent with a rate of 0.14$\pm$0.05 nm/hour. We show that the life-time of the GaSe films can be increased by up to two orders of magnitude (to several months) by encapsulation in dielectric materials such as SiO$_2$ or Si$_x$N$_y$.

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arXiv2015

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.

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arXiv2015

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.

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arXiv2014

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.

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arXiv2014

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↗

arXiv2014

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).

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arXiv2014

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↗

arXiv2013

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.

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arXiv2012

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.

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arXiv2012

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↗

arXiv2011

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.

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arXiv2011

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↗

arXiv2010

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.

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