Coherent Hole Research Articles

Sweet-spot operation of a germanium hole spin qubit with highly anisotropic noise sensitivity

Spin qubits defined by valence band hole states are attractive for quantum information processing due to their inherent coupling to electric fields, enabling fast and scalable qubit control. Heavy holes in germanium are particularly promising, with recent demonstrations of fast and high-fidelity qubit operations. However, the mechanisms and anisotropies that underlie qubit driving and decoherence remain mostly unclear. Here we report the highly anisotropic heavy-hole g-tensor and its dependence on electric fields, revealing how qubit driving and decoherence originate from electric modulations of the g-tensor. Furthermore, we confirm the predicted Ising-type hyperfine interaction and show that qubit coherence is ultimately limited by 1/f charge noise, where f is the frequency. Finally, operating the qubit at low magnetic field, we measure a dephasing time of T2*\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$${T}_{2}^{* }$$\\end{document} = 17.6 μs, maintaining single-qubit gate fidelities well above 99% even at elevated temperatures of T > 1 K. This understanding of qubit driving and decoherence mechanisms is key towards realizing scalable and highly coherent hole qubit arrays.

Observation of quadrupolar and dipolar excitons in a semiconductor heterotrilayer.

Van der Waals (vdW) materials have opened up many avenues for discovery through layer assembly, as epitomized by interlayer dipolar excitons that exhibit electrically tunable luminescence, lasing and exciton condensation. Extending interlayer excitons to more vdW layers, however, raises fundamental questions concerning coherence within excitons and coupling between moiré superlattices at multiple interfaces. Here, by assembling angle-aligned WSe2/WS2/WSe2 heterotrilayers, we demonstrate the emergence of quadrupolar excitons. We confirm the exciton's quadrupolar nature by the decrease in its energy of 12 meV from coherent hole tunnelling between the two outer layers, its tunable static dipole moment under an external electric field and the reduced exciton-exciton interactions. At high exciton density, we also see signatures of a phase of oppositely aligned dipolar excitons, consistent with a staggered dipolar phase predicted to be driven by attractive dipolar interactions. Our demonstration paves the way for discovering emergent exciton orderings for three vdW layers and beyond.

Constructing hole transport channels in the photoactive layer connecting dopant-free hole transport layers to improve the power conversion efficiency of perovskite solar cells

Perovskite solar cells (PSCs) with dopant‐free hole transporting layers (HTLs) deserved extensive research by merits of their outstanding hydrophobicity and stability. However, the low carrier mobility and poor interfacial hole extraction lead to the inferior power conversion efficiency (PCE) than that of conventional Li+ doped Spiro-OMeTAD. Here, a design of triphenylamine groups grafted triphenylene derivative (T-6TPA) as dopant-free HTLs has been presented. The larger π-conjugation in T-6TPA give rise to high hole mobility of 2.06 × 10−3 cm2V−1s−1. Moreover, the interfacial hole extraction of T-6TPA was significantly promoted when the molecules were infiltrated into perovskite before HTL deposition. The infiltration method of anti-solvent dripping (An) strategy increased PCE from 18.5% up to 20.3%, which is superior to another additive doping strategy (Ad-strategy, 19.3%). The effectiveness of An-strategy can be attributed to the construction of a coherent and homogeneous hole transport channel. The hydrophobicity and high glass transition temperature of T-6TPA also granted excellent moisture and thermal stabilities that the initial PCE could remain 80% for 60 days in air or 600 h at 60 °C. This work highlights the synergistical optimization by design of highly hole-mobile materials as well as the interfacial network construction for charge transport.

Laser-Induced Hole Coherence and Spatial Self-Phase Modulation in the Anisotropic 3D Weyl Semimetal TaAs.

Laser-induced electron coherence is a fascinating topic in manipulating quantum materials. Recently, it has been shown that laser-induced electron coherence in 2D materials can produce a third-order nonlinear optical response spatial self-phase modulation (SSPM), which has been used to develop a novel all-optical switching scheme. However, such investigations have mainly focused on electron coherence, whereas laser-induced hole coherence is rarely explored. Here, the observation of the optical Kerr effect in 3D Weyl semimetal TaAs flakes is reported. The nonlinear susceptibility (χ(3) ) is obtained, which exhibits a surprisingly high value (with = 9.9×10-9 e.s.u. or 1.4×10-16 m2 V-2 at 532nm). This cannot be explained by the conventional electron mobility, but can be well understood by the unique high anisotropic hole mobility of TaAs. The wind-chime model and χ(3) carrier mobility correlation adequately explain the results, suggesting the crucial role of laser-induced nonlocal ac hole coherence. These observations extend the understanding of SSPM from 2D to 3D quantum materials with anisotropic carrier mobility and from electron coherence to hole coherence.

Strong non-linear optical response of Sb2Se3 nanorods in a liquid suspension based on spatial self-phase modulation and their all-optical photonic device applications.

The field of nonlinear optics is constantly expanding and gaining new impetus through the discovery of fresh nonlinear materials. Herein, for the first time, we have performed spatial self-phase modulation (SSPM) experiments with an emerging anisotropic Sb2Se3 layered material in a liquid suspension for an all-optical diode and all-optical switching application. The third-order broadband nonlinear optical susceptibility (χ(3)single layer ∼ 10-9 esu) and nonlinear refractive index (n2 ∼ 10-6 cm2 W-1) of Sb2Se3 have been determined using a 671 nm laser beam. This result could be unambiguously explained by the anisotropic hole mobility of Sb2Se3. The linear relationship of χ(3) and carrier mobility emphasizes the establishment of nonlocal hole coherence, the origin of the diffraction pattern. Consequently, the time evolution of diffraction rings follows the 'Wind-Chime' model. A novel photonic diode based on Sb2Se3/SnS2 has been demonstrated using the nonreciprocal propagation of light. The self-phase modulation (SPM) technique uses laser lights of different wavelengths and intensities to demonstrate the all-optical logic gates, particularly OR logic gates. The exploration of nonlinear optical phenomena in Sb2Se3 opens up a new realm for optical information processing and communication. We strongly believe that this result will help to underpin the area of optical nonlinearities among its various applications.

Geometry and thermodynamics of coherent quantum black holes

In this paper, we present a quantum description of black holes given by coherent states of gravitons sourced by a matter core. The expected behavior in the weak-field region outside the horizon is recovered, with arbitrarily good approximation, but the classical central singularity is not resolved because the coherent states may not contain modes of arbitrarily short wavelength and the matter core must therefore have finite size. Ensuing quantum corrections both in the interior and exterior is also estimated by assuming that the mean-field approximation holds everywhere. These deviations from the classical black hole geometry can be viewed as quantum hair and will lead to a quantum corrected horizon radius and thermodynamics.

Doped Mott insulators in the triangular-lattice Hubbard model

We investigate the evolution of the Mott insulators in the triangular lattice Hubbard Model, as a function of hole doping $\delta$ in both the strong and intermediate coupling limits. Using the advanced density matrix renormalization group (DMRG) method, at light hole doping $\delta\lesssim 10\%$, we find a significant difference between strong and intermediate couplings. Notably, at intermediate coupling an unusual metallic state emerges, with short ranged spin correlations but long ranged spin-chirality order. Moreover, no clear Fermi surface or wave-vector is observed, this chiral metal also exhibits staggered loop current, which breaks the translational symmetry. These features disappear on increasing interaction strength or on further doping. At strong coupling, the 120 degree magnetic order of the insulating magnet persists for light doping, and produces hole pockets with a well defined Fermi surface. On further doping, $\delta \approx 10\%\sim 20\%$ SDW order and coherent hole Fermi pockets are found at both strong and intermediate couplings. At even higher doping $\delta \gtrsim 20\%$, the SDW order is suppressed and the spin-singlet Cooper pair correlations are simultaneously enhanced. We also briefly comment on the strong particle-hole asymmetry of the model.

Coherent Surface Plasmon Hole Burning via Spontaneously Generated Coherence.

Surface plasmon (SP)—induced spectral hole burning (SHB) at the silver-dielectric interface is investigated theoretically. We notice a typical lamb dip at a selective frequency, which abruptly reduces the absorption spectrum of the surface plasmons polaritons (SPP). Introducing the spontaneous generated coherence (SGC) in the atomic medium, the slope of dispersion becomes normal. Additionally, slow SPP propagation is also noticed at the interface. The spectral hole burning dip is enhanced with the SGC effect and can be modified and controlled with the frequency and intensity of the driving fields. The SPP propagation length at the hole-burning region is greatly enhanced under the effect of SGC. A propagation length of the order of 600 µm is achieved for the modes, which is a remarkable result. The enhancement of plasmon hole burning under SGC will find significant applications in sensing technology, optical communication, optical tweezers and nano-photonics.

Energy Tuning of Electronic Spin Coherent Evolution in Methylammonium Lead Iodide Perovskites.

We investigated the coherent evolution of the electronic spin at low temperature in high-quality CH3NH3PbI3 polycrystalline films by picosecond-resolved photoinduced Faraday rotation. We show that this coherent evolution can be tuned by choosing the pump-probe energy within the lowest optical-absorption band, and we explain it as the result of two main contributions: the localized electron and the localized hole. Their corresponding amplitude ratios are not constant across the lowest absorption band-an observation which disqualifies a free exciton from being at the origin of the electronic spin coherent evolution. We measured a spin coherence time of localized electrons (holes) of 4.4 ns (3.7 ns) at 1.635 eV, which evolves to about 7 ns at 1.612 eV (the hole coherence time remains almost constant at lower energies). Finally, we provide a global image of the spin coherent evolution in bulk metal halide perovskite, which overcomes recent controversies.

Coherent Spin Precession and Lifetime-Limited Spin Dephasing in CsPbBr3 Perovskite Nanocrystals.

Carrier spins in semiconductor nanocrystals are promising candidates for quantum information processing. Using a combination of time-resolved Faraday rotation and photoluminescence spectroscopies, we demonstrate optical spin polarization and coherent spin precession in colloidal CsPbBr3 nanocrystals that persists up to room temperature. By suppressing the influence of inhomogeneous hyperfine fields with a small applied magnetic field, we demonstrate inhomogeneous hole transverse spin-dephasing times (T2*) that approach the nanocrystal photoluminescence lifetime, such that nearly all emitted photons derive from coherent hole spins. Thermally activated LO phonons drive additional spin dephasing at elevated temperatures, but coherent spin precession is still observed at room temperature. These data reveal several major distinctions between spins in nanocrystalline and bulk CsPbBr3 and open the door for using metal-halide perovskite nanocrystals in spin-based quantum technologies.

Fermi surface electron–hole instability of the (TMTSF)2PF6 Bechgaard salt revealed by the first-principles Lindhard response function

We report the first-principles DFT calculation of the electron–hole Lindhard response function of the (TMTSF)2PF6 Bechgaard salt using the real triclinic low-temperature structure. The Lindhard response is found to change considerably with temperature. Near the 2kF spin density wave (SDW) instability it has the shape of a broad triangular plateau as a result of the multiple nesting associated with the warped quasi-one-dimensional Fermi surface. The evolution of the 2kF broad maximum as well as the effect of pressure and deuteration is calculated and analyzed. The thermal dependence of the electron–hole coherence length deduced from these calculations compares very well with the experimental thermal evolution of the 2kF bond order wave correlation length. The existence of a triangular plateau of maxima in the low-temperature electron–hole Lindhard response of (TMTSF)2PF6 should favor a substantial mixing of q-dependent fluctuations which can have important consequences in understanding the phase diagram of the 2kF SDW ground state, the mechanism of superconductivity and the magneto-transport of this paradigmatic quasi-one-dimensional material. The first-principles DFT Lindhard response provides a very accurate and unbiased approach to the low-temperature instabilities of (TMTSF)2PF6 which can take into account in a simple way 3D effects and subtle structural variations, thus providing a very valuable tool in understanding the remarkable physics of molecular conductors.

Coherent spectral hole burning and qubit isolation by stimulated Raman adiabatic passage

We describe how stimulated Raman adiabatic passage (STIRAP) can be applied to create spectral holes in an inhomogeneously broadened system. Due to the robustness of STIRAP, our proposal guarantees high flexibility and accuracy and, at variance with traditional spectral hole burning techniques, it may require substantially less time resources since it does not rely upon the spontaneous decay of an intermediate excited state. We investigate the effects on the scheme of dephasing and dissipation as well as of unintentional driving of undesired transitions due to a finite splitting of the initial and target state. Finally, we show that the pulses can be reversed to create narrow absorption structures inside a broad spectral hole, which can be used as qubits for precise quantum operations on inhomogeneously broadened few-level systems.

Visualization of Photoinduced Charge Transfer and Electron–Hole Coherence in Two-Photon Absorption

We provide a visualization method to observe the photoinduced charge transfer and electron–hole coherence in the two-photon absorption (TPA), especially including the optical properties in the “hid...

A germanium hole spin qubit

Holes confined in quantum dots have gained considerable interest in the past few years due to their potential as spin qubits. Here we demonstrate two-axis control of a spin 3/2 qubit in natural Ge. The qubit is formed in a hut wire double quantum dot device. The Pauli spin blockade principle allowed us to demonstrate electric dipole spin resonance by applying a radio frequency electric field to one of the electrodes defining the double quantum dot. Coherent hole spin oscillations with Rabi frequencies reaching 140 MHz are demonstrated and dephasing times of 130 ns are measured. The reported results emphasize the potential of Ge as a platform for fast and electrically tunable hole spin qubit devices.

Coherence of a dynamically decoupled quantum-dot hole spin

A heavy hole confined to an InGaAs quantum dot promises the union of a stable spin and optical coherence to form a near perfect, high-bandwidth spin-photon interface. Despite theoretical predictions and encouraging preliminary measurements, the dynamic processes determining the coherence of the hole spin are yet to be understood. Here, we establish the regimes that allow for a highly coherent hole spin in these systems, recovering a crossover from hyperfine to electrical-noise dominated decoherence with a few-Tesla external magnetic field. Dynamical decoupling allows us to reach the longest ground-state coherence time, T2, of 4.4 $\mu$s, observed in this system. The improvement of coherence we measure is quantitatively supported by an independent analysis of the local electrical environment.

Formation of electron holes in the long-time evolution of the bump-on-tail instability

AbstractAn Eulerian Vlasov code is applied for the numerical solution of the one-dimensional Vlasov–Poisson system of equations for electrons, and with ions forming an immobile background. We study the non-linear evolution of the bump-on-tail instability in the case when the system length L is greater than the wavelength λ of the unstable mode, with a beam density of 10% of the total density, nb = 0.1. We follow the growth and the saturation of an initially unstable wave perturbation, and the formation of a traveling Bernstein–Greene–Kruskal (BGK) mode, which evolves out of the instability. This first stage is followed by sidebands growing from round-off errors which develop and disrupt the BGK equilibrium. In the excited spectrum, mode coupling is mediated by the oscillating resonant particles and results in the electric energy of the system flowing to the longest wavelengths (inverse cascade), and reaching in the asymptotic state a steady state with constant amplitude oscillation modulated by the persistent oscillation of the trapped particles. Coherent phase-space electron holes are formed, which are localized phase-space regions of reduced density on trapped electron orbits, where the electron density is lower than the surrounding plasma electron density. The distribution function evolves to a shape with stationary inflection points of zero slope, at the phase velocities of the excited waves. The longest wavelengths show oscillations at frequencies below the plasma frequency, with phase velocities higher than that of the injected beam, which can accelerate electrons to energies in excess of the initial beam energy. The present work makes a connection between the formation of electron holes, the existence of inflection points of zero slopes in the electron distribution function at the phase velocities of the dominant waves, and at frequencies below the plasma frequency. A fine resolution grid is used in the Eulerian Vlasov code in the phase space and time to allow an accurate calculation of the time history of the system and of the dynamic and oscillation of the trapped particles in the low-density regions of the phase space, and of those particles at the separatrix regions of the vortex structures which evolve periodically between trapping and untrapping states and which can only be accurately studied using a fine-resolution phase-space grid.

Effect of the reflectional symmetry on the coherent hole transport across DNA hairpins.

The coherent hole transfer in three types of DNA hairpins containing strands with adenine (A) and guanine (G) nucleobases has been studied. The investigated hairpins involve An+1GGAn, AnGAGAn, or (AG)2nA strands that connect the hole donor and hole acceptor located on opposite ends of hairpins. The positive charge transfer from the photo-excited donor to the acceptor is shown to be slower for An+1GGAn in comparison with AnGAGAn and (AG)2nA sequences. We have revealed that this is due to the reflectional symmetry of the last two sequences with respect to the axis passing through the middle base. As has been demonstrated, the symmetry of the sequence structure manifests itself in the reflectional symmetry of the energy eigenstates. In addition, it has been shown that (AG)2nA is the only symmetric sequence with a zero energy state in the middle of the LUMO tight-binding energy band. Based on our theoretical findings, we predict that the hairpin with this sequence should have the fastest coherent hole transfer rate among the class of base sequences studied.

Role of phase space structures in collisionless drift wave turbulence and impact on transport modeling

In fusion plasmas, several mechanisms such as heating, wave-particle interaction etc can drive deviations of distribution function from Maxwelian to form phase space structures. This article discusses the impact of phase space structures in drift wave turbulence on dynamics and transport modeling. The two cases of (i) coherent holes and (ii) incoherent granulations (clusters of correlated resonant particles with finite life time) are treated. Their dynamical impact on driving subcritical instability is analyzed by explicitly calculating the nonlinear growth rate. The role of zonal flows is also addressed. It is explained how phase space structures can be related to transient events and non-diffusive transport, issues in current confinement research.

Coherent hole propagation in an exactly solvable gapless spin liquid

We examine the dynamics of a single hole in the gapless phase of the Kitaev honeycomb model, focusing on the slow-hole regime where the bare hopping amplitude $t$ is much less than the Kitaev exchange energy $J$. In this regime, the hole does not generate gapped flux excitations and is dressed only by the gapless fermion excitations. Investigating the single-hole spectral function, we find that the hole propagates coherently with a quasiparticle weight that is finite but approaches zero as $t/J \to 0$. This conclusion follows from two approximate treatments, which capture the same physics in complementary ways. Both treatments use the stationary limit as an exactly solvable starting point to study the spectral function approximately (i) by employing a variational approach in terms of a trial state that interpolates between the limits of a stationary hole and an infinitely fast hole and (ii) by considering a special point in the gapless phase that corresponds to a simplified one-dimensional problem.

Maximizing hole coherence in ultrafast photoionization of argon with an optimization by sequential parametrization update

Photoionization with attosecond pulses populates hole states in the photoion. Superpositions of hole states represent ideal candidates for time-dependent spectroscopy, for example via pump-probe studies. The challenge consists in identifying pulses that create coherent superpositions of hole states while satisfying practical constraints. Here, we employ quantum optimal control to maximize the degree of coherence between these hole states. To this end, we introduce a derivative-free optimization method with Sequential PArametrization update (SPA-optimization). We demonstrate the versatility and computational efficiency of SPA-optimization for photoionization in argon by maximizing the coherence between the $3s$ and $3p_0$ hole states using shaped attosecond pulses. We show that it is possible to maximize the hole coherence while simultaneously prescribing the ratio of the final hole state populations.