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Pauli blockade is a fundamental quantum phenomenon that also serves as a powerful tool for qubit manipulation and read-out. While most systems exhibit a simple even-odd pattern of double-dot Pauli spin blockade due to the preferred singlet pairing of spins, the additional valley degree of freedom offered by bilayer graphene greatly alters this pattern. Inspecting bias-triangle measurements at double-dot charge degeneracies with up to four electrons in each dot reveals a much richer double-dot Pauli blockade catalogue with both spin and/or valley blockade. In addition, we use single-dot Kondo effect measurements to substantiate our understanding of the three- and four-particle state spectra by analyzing their magnetic field dependence. With high controllability and reported long valley- and spin-relaxation times, bilayer graphene is a rising platform for hosting semiconductor quantum dot qubits. A thorough understanding of state spectra is crucial for qubit design and manipulation, and the rich Pauli blockade catalogue provides an abundance of novel qubit operational possibilities and opportunities to explore intriguing spin and valley physics., Comment: 11 pages, 6 figures

The spin degree of freedom is crucial for the understanding of any condensed matter system. Knowledge of spin-mixing mechanisms is not only essential for successful control and manipulation of spin-qubits, but also uncovers fundamental properties of investigated devices and material. For electrostatically-defined bilayer graphene quantum dots, in which recent studies report spin-relaxation times T1 up to 50ms with strong magnetic field dependence, we study spin-blockade phenomena at charge configuration $(1,2)\leftrightarrow(0,3)$. We examine the dependence of the spin-blockade leakage current on interdot tunnel coupling and on the magnitude and orientation of externally applied magnetic field. In out-of-plane magnetic field, the observed zero-field current peak could arise from finite-temperature co-tunneling with the leads; though involvement of additional spin- and valley-mixing mechanisms are necessary for explaining the persistent sharp side peaks observed. In in-plane magnetic field, we observe a zero-field current dip, attributed to the competition between the spin Zeeman effect and the Kane-Mele spin-orbit interaction. Details of the line shape of this current dip however, suggest additional underlying mechanisms are at play.

We measure telegraph noise of current fluctuations in an electrostatically defined quantum dot in bilayer graphene by real-time detection of single electron tunneling with a capacitively coupled neighboring quantum dot. Suppression of the second and third cumulant (related to shot noise) in a tunable graphene quantum dot is demonstrated experimentally. With this method we demonstrate the ability to measure very low current and noise levels. Furthermore, we use this method to investigate the first spin excited state, an essential prerequisite to measure spin relaxation.

Bilayer graphene is a nanomaterial that allows for well-defined, separated quantum states to be defined by electrostatic gating and, therefore, provides an attractive platform to construct tunable quantum dots. When a magnetic field perpendicular to the graphene layers is applied, the graphene valley degeneracy is lifted, and splitting of the energy levels of the dot is observed. Given the experimental ability to engineer this energy valley splitting, bilayer graphene quantum dots have a great potential for hosting robust qubits. Although bilayer graphene quantum dots have been recently realized in experiments, it is critically important to devise robust methods that can identify the observed quantum states from accessible measurement data. Here, we develop an efficient algorithm for extracting the model parameters needed to characterize the states of a bilayer graphene quantum dot completely. We introduce a Hamiltonian-guided random search method and demonstrate robust identification of quantum states on both simulated and experimental data., Comment: 18 pages, 17 figures, code: https://gitlab.com/QMAI/papers/bilayergrapheneqds

Electrostatically defined quantum dots in bilayer graphene offer a promising platform for spin qubits with presumably long coherence times due to low spin-orbit coupling and low nuclear spin density. We demonstrate two different experimental approaches to measure the decay times of excited states. The first is based on direct current measurements through the quantum device. Pulse sequences are applied to control the occupation of ground and excited states. We observe a lower bound for the excited state decay on the order of hundred microseconds. The second approach employs a capacitively coupled charge sensor to study the time dynamics of the excited state using the Elzerman technique. We find that the relaxation time of the excited state is of the order of milliseconds. We perform single-shot readout of our two-level system with a visibility of $87.1\%$, which is an important step for developing a quantum information processor in graphene.

Single electron tunneling and its transport statistics have been studied for some time using high precision charge detectors. However, this type of detection requires advanced lithography, optimized material systems and low temperatures (mK). A promising alternative, recently demonstrated, is to exploit an optical transition that is turned on or off when a tunnel event occurs. High bandwidths should be achievable with this approach, although this has not been adequately investigated so far. We have studied low temperature resonance fluorescence from a self-assembled quantum dot embedded in a diode structure. We detect single photons from the dot in real time and evaluate the recorded data only after the experiment, using post-processing to obtain the random telegraph signal of the electron transport. This is a significant difference from commonly used charge detectors and allows us to determine the optimal time resolution for analyzing our data. We show how this post-processing affects both the determination of tunneling rates using waiting-time distributions and statistical analysis using full-counting statistics. We also demonstrate, as an example, that we can analyze our data with bandwidths as high as 350 kHz. Using a simple model, we discuss the limiting factors for achieving the optimal bandwidth and propose how a time resolution of more than 1 MHz could be achieved., Comment: 8 pages, 4 figures

Time-resolved studies of quantum systems are the key to understand quantum dynamics at its core. The real-time measurement of individual quantum numbers as they switch between certain discrete values, well known as random telegraph signal, is expected to yield maximal physical insight. However, the signal suffers from both systematic errors, such as a limited time resolution and noise from the measurement apparatus, as well as statistical errors due to a limited amount of data. Here we demonstrate that an evaluation scheme based on factorial cumulants can reduce the influence of such errors by orders of magnitude. The error resilience is supported by a general theory for the detection errors as well as experimental data of single-electron tunnelling through a self-assembled quantum dot. Thus, factorial cumulants push the limits in the analysis of random telegraph data which represent a wide class of experiments in physics, chemistry, engineering and life sciences., Comment: 7 pages manuscript + 16 pages supplementary information

Pauli blockade mechanisms -- whereby carrier transport through quantum dots is blocked due to selection rules even when energetically allowed -- are a direct manifestation of the Pauli exclusion principle, as well as a key mechanism for manipulating and reading out spin qubits. Pauli spin blockade is well established for systems such as GaAs QDs, but is to be further explored for systems with additional degrees of freedom, such as the valley quantum numbers in carbon-based materials or silicon. Here we report experiments on coupled bilayer graphene double quantum dots, in which the spin and valley states are precisely controlled, enabling the observation of the two-electron combined blockade physics. We demonstrate that the doubly occupied single dot switches between two different ground states with gate and magnetic-field tuning, allowing for the switching of selection rules: with a spin-triplet--valley-singlet ground state, valley-blockade is observed; and with the spin-singlet--valley-triplet ground state, robust spin blockade is shown.

The Kondo effect is a cornerstone in the study of strongly correlated fermions. The coherent exchange coupling of conduction electrons to local magnetic moments gives rise to a Kondo cloud that screens the impurity spin. Whereas complete Kondo screening has been explored widely, realizations of the underscreened scenario - where only some of several Kondo channels participate in the screening - remain rare. Here we report the observation of fully screened and underscreened Kondo effects in quantum dots in bilayer graphene. More generally, we introduce a unique platform for studying Kondo physics. In contrast to carbon nanotubes, whose curved surfaces give rise to strong spin-orbit coupling breaking the SU(4) symmetry of the electronic states relevant for the Kondo effect, we study a nominally flat carbon material with small spin-orbit coupling. Moreover, the unusual two-electron triplet ground state in bilayer graphene dots provides a route to exploring the underscreened spin-1 Kondo effect.

Transport measurements through a few-electron circular quantum dot in bilayer graphene display bunching of the conductance resonances in groups of four, eight and twelve. This is in accordance with the spin and valley degeneracies in bilayer graphene and an additional threefold 'minivalley degeneracy' caused by trigonal warping. For small electron numbers, implying a small dot size and a small displacement field, a two-dimensional s- and then a p-shell are successively filled with four and eight electrons, respectively. For electron numbers larger than twelve, as the dot size and the displacement field increase, the single-particle ground state evolves into a three-fold degenerate minivalley ground state. A transition between these regimes is observed in our measurements and can be described by band-structure calculations. Measurements in magnetic field confirm Hund's second rule for spin filling of the quantum dot levels, emphasizing the importance of exchange interaction effects., Comment: 10 pages, 7 figures

We demonstrate by time-resolved resonance fluorescence measurements on a single self-assembled quantum dot an internal photo-effect that emits electrons from the dot by an intra-band excitation. We find a linear dependence of the optically generated emission rate on the excitation intensity and use a rate equation model to deduce the involved rates. The emission rate is tunable over several orders of magnitude by adjusting the excitation intensity. Our findings show that a process that is well known in single atom spectroscopy (i.e. photo ionization) can also be observed in the solid state. The results also quantify an important, but mostly neglected, mechanism that may fundamentally limit the coherence times in solid-state quantum optical devices., Comment: 4 pages, 3 figures

Quantum states in graphene are four-fold degenerate: two fold in spins, and two fold in valleys.Both degrees of freedom can be utilized for qubit preparations. In our bilayer graphene quantumdots, we demonstrate that the valley g-factorgv, defined analogously as the spin g-factorgsforvalley splitting in perpendicular magnetic field, is tunable by over a factor of 4 from 20 to 90. Wefind that largergvresults from larger electronic dot sizes, determined from the charging energy.This control is achieved by adjusting voltages on merely two gates, which also allows for tuning ofthe dot-lead tunnel coupling. On our versatile device, bipolar operation, charging our quantum dotwith charge carriers of the same or the opposite polarity as the leads, can be performed. Dots ofboth polarity are tunable to the first charge carrier by action of the plunger gate, such that thetransition from an electron to a hole dot can be observed. By adding more gates, this system caneasily be extended to host double dots., Comment: 10 pages, 7 figures

Graphene has evolved as a platform for quantum transport that can compete with the best and cleanest semiconductor systems. Recently, many interesting local properties of carrier transport in graphene have been investigated by various scanning probe techniques. Here, we report on the observation of distinct electronic jets emanating from a narrow split-gate defined channel in bilayer graphene. We find that these jets, which are visible via their interference patterns, occur predominantly with an angle of 60{\deg} between each other. This observation is related to the specific bandstructure of bilayer graphene, in particular trigonal warping, which leads to a valley-dependent selection of momenta for low-energy conduction channels. This experimental observation of electron jetting has consequences for carrier transport in graphene in general as well as for devices relying on ballistic and valley selective transport.

We use Scanning Gate Microscopy to demonstrate the presence of localized states arising from potential inhomogeneities in a 50nm-wide, gate-defined conducting channel in encapsulated bilayer graphene. When imaging the channel conductance under the influence of a local tip-induced potential, we observe ellipses of enhanced conductance as a function of the tip position. These ellipses allow us to infer the location of the localized states and to study their dependence on the displacement field. For large displacement fields, we observe that localized states tend to occur halfway into the channel. All our observations can be well explained within the framework of stochastic Coulomb blockade.

When twisted to angles near 1{\deg}, graphene multilayers provide a new window on electron correlation physics by hosting gate-tuneable strongly-correlated states, including insulators, superconductors, and unusual magnets. Here we report the discovery of a new member of the family, density-wave states, in double bilayer graphene twisted to 2.37{\deg}. At this angle the moir\'e states retain much of their isolated bilayer character, allowing their bilayer projections to be separately controlled by gates. We use this property to generate an energetic overlap between narrow isolated electron and hole bands with good nesting properties. Our measurements reveal the formation of ordered states with reconstructed Fermi surfaces, consistent with density-wave states, for equal electron and hole densities. These states can be tuned without introducing chemical dopants, thus opening the door to a new class of fundamental studies of density-waves and their interplay with superconductivity and other types of order, a central issue in quantum matter physics.

Control over minivalley polarization and interlayer coupling is demonstrated in double bilayer graphene twisted with an angle of 2.37$^\circ$. This intermediate angle is small enough for the minibands to form and large enough such that the charge carrier gases in the layers can be tuned independently. Using a dual-gated geometry we identify and control all possible combinations of minivalley polarization via the population of the two bilayers. An applied displacement field opens a band gap in either of the two bilayers, allowing us to even obtain full minivalley polarization. In addition, the wavefunctions of the minivalleys are mixed by tuning through a Lifshitz transition, where the Fermi surface topology changes. The high degree of control makes twisted double bilayer graphene a promising platform for valleytronics devices such as valley valves, filters and logic gates., Comment: Supplemental Material included in PDF

In multivalley semiconductors, the valley degree of freedom can be potentially used to store, manipulate and read quantum information, but its control remains challenging. The valleys in bilayer graphene can be addressed by a perpendicular magnetic field which couples by the valley g-factor. However, control over the valley g-factor has not been demonstrated yet. We experimentally determine the energy spectrum of a quantum point contact realized by a suitable gate geometry in bilayer graphene. Using finite bias spectroscopy we measure the energy scales arising from the lateral confinement as well as the Zeeman splitting and find a spin g-factor of 2. The valley g-factor can be tuned by a factor of 3 using vertical electric fields, reaching values between 40 and 120. The results are quantitatively explained by a calculation considering topological magnetic moment and its dependence on confinement and the vertical displacement field.

Auger recombination is a non-radiative process, where the recombination energy of an electron-hole pair is transferred to a third charge carrier. It is a common effect in colloidal quantum dots that quenches the radiative emission with an Auger recombination time below nanoseconds. In self-assembled QDs, the Auger recombination has been observed with a much longer recombination time in the order of microseconds. Here, we use two-color laser excitation on the exciton and trion transition in resonance fluorescence on a single self-assembled quantum dot to monitor in real-time every quantum event of the Auger process. Full counting statistics on the random telegraph signal give access to the cumulants and demonstrate the tunability of the Fano factor from a Poissonian to a sub-Poissonian distribution by Auger-mediated electron emission from the dot. Therefore, the Auger process can be used to tune optically the charge carrier occupation of the dot by the incident laser intensity; independently from the electron tunneling from the reservoir by the gate voltage. Our findings are not only highly relevant for the understanding of the Auger process, it also demonstrates the perspective of the Auger effect for controlling precisely the charge state in a quantum system by optical means., Comment: 17 pages

Thin nanomaterials are key constituents of modern quantum technologies and materials research. Identifying specimens of these materials with properties required for the development of state of the art quantum devices is usually a complex and lengthy human task. In this work we provide a neural-network driven solution that allows for accurate and efficient scanning, data-processing and sample identification of experimentally relevant two-dimensional materials. We show how to approach classification of imperfect imbalanced data sets using an iterative application of multiple noisy neural networks. We embed the trained classifier into a comprehensive solution for end-to-end automatized data processing and sample identification., Comment: 8 pages, 4 figures

Crystal fields occur due to a potential difference between chemically different atomic species. In Van-der-Waals heterostructures such fields are naturally present perpendicular to the planes. It has been realized recently that twisted graphene multilayers provide powerful playgrounds to engineer electronic properties by the number of layers, the twist angle, applied electric biases, electronic interactions and elastic relaxations, but crystal fields have not received the attention they deserve. Here we show that the bandstructure of large-angle twisted double bilayer graphene is strongly modified by crystal fields. In particular, we experimentally demonstrate that twisted double bilayer graphene, encapsulated between hBN layers, exhibits an intrinsic bandgap. By the application of an external field, the gaps in the individual bilayers can be closed, allowing to determine the crystal fields. We find that crystal fields point from the outer to the inner layers with strengths in the bottom (top) bilayer of -0.13 V/nm (0.12 V/nm). We show both by means of first principles calculations and low energy models that crystal fields open a band gap in the groundstate. Our results put forward a physical scenario in which a crystal field effect in carbon substantially impacts the low energy properties of twisted double bilayer graphene, suggesting that such contributions must be taken into account in other regimes to faithfully predict the electronic properties of twisted graphene multilayers.

Efficient and versatile spin-to-charge current conversion is crucial for the development of spintronic applications, which strongly rely on the ability to electrically generate and detect spin currents. In this context, the spin Hall effect has been widely studied in heavy metals with strong spin-orbit coupling. While the high crystal symmetry in these materials limits the conversion to the orthogonal configuration, unusual configurations are expected in low symmetry transition metal dichalcogenide semimetals, which could add flexibility to the electrical injection and detection of pure spin currents. Here, we report the observation of spin-to-charge conversion in MoTe$_2$ flakes, which are stacked in graphene lateral spin valves. We detect two distinct contributions arising from the conversion of two different spin orientations. In addition to the conventional conversion where the spin polarization is orthogonal to the charge current, we also detect a conversion where the spin polarization and the charge current are parallel. Both contributions, which could arise either from bulk spin Hall effect or surface Edelstein effect, show large efficiencies comparable to the best spin Hall metals and topological insulators. Our finding enables the simultaneous conversion of spin currents with any in-plane spin polarization in one single experimental configuration., Comment: 14 pages, 4 figures, and Supporting Information

The van-der-Waals stacking technique enables the fabrication of heterostructures, where two conducting layers are atomically close. In this case, the finite layer thickness matters for the interlayer electrostatic coupling. Here we investigate the electrostatic coupling of two graphene layers, twisted by 22 degrees such that the layers are decoupled by the huge momentum mismatch between the K and K' points of the two layers. We observe a splitting of the zero-density lines of the two layers with increasing interlayer energy difference. This splitting is given by the ratio of single-layer quantum capacitance over interlayer capacitance C and is therefore suited to extract C. We explain the large observed value of C by considering the finite dielectric thickness d of each graphene layer and determine d=2.6 Angstrom. In a second experiment we map out the entire density range with a Fabry-P\'erot resonator. We can precisely measure the Fermi-wavelength in each layer, showing that the layers are decoupled. We find that the Fermi wavelength exceeds 600nm at the lowest densities and can differ by an order of magnitude between the upper and lower layer. These findings are reproduced using tight-binding calculations.

Electrostatic confinement of charge carriers in bilayer graphene provides a unique platform for carbon-based spin, charge or exchange qubits. By exploiting the possibility to induce a band gap with electrostatic gating, we form a versatile and widely tunable multi-quantum dot system. We demonstrate the formation of single, double and triple quantum dots that are free of any sign of disorder. In bilayer graphene we have the possibility to form tunnel barriers using different mechanisms. We can exploit the ambipolar nature of bilayer graphene where pn-junctions form natural tunnel barriers. Alternatively, we can use gates to form tunnel barriers, where we can vary the tunnel coupling by more than two orders of magnitude tuning between a deeply Coulomb blockaded system and a Fabry-P\'erot-like cavity. Demonstrating such tunability is an important step towards graphene-based quantum computation., Comment: 8 pages, 5 figures

In bilayer graphene, electrostatic confinement can be realized by a suitable design of top and back gate electrodes. We measure electronic transport through a bilayer graphene quantum dot, which is laterally confined by gapped regions and connected to the leads via p-n junctions. Single electron and hole occupancy is realized and charge carriers $n = 1, 2,\dots 50$ can be filled successively into the quantum system with charging energies exceeding $10 \ \mathrm{meV}$. For the lowest quantum states, we can clearly observe valley and Zeeman splittings with a spin g-factor of $g_{s}\approx 2$. In the low field-limit, the valley splitting depends linearly on the perpendicular magnetic field and is in qualitative agreement with calculations., Comment: 7 pages, 4 figures

Time-resolved resonance fluorescence (RF) on a single self-assembled quantum dot (QD) is used to analyze the generation and capture of photoinduced free charge carriers. We directly observe the capture of electrons into the QD in an intensity reduction of the exciton transition. The exciton transition is quenched until the captured electron tunnels out of the dot again in the order of milliseconds. Our results demonstrate that even under resonant excitation, excited, free electrons are generated, which can negatively influence the optical properties of a QD. This detrimental effect has been neglected before for dots that are optimized for maximum efficiency and minimum spectral diffusion.

In quantum dots (QDs) the Auger recombination is a non-radiative process, where the electron-hole recombination energy is transferred to an additional carrier. It has been studied mostly in colloidal QDs, where the Auger recombination time is in the ps range and efficiently quenches the light emission. In self-assembled QDs, on the other hand, the influence of Auger recombination on the optical properties is in general neglected, assuming that it is masked by other processes such as spin and charge fluctuations. Here, we use time-resolved resonance fluorescence to analyze the Auger recombination and its influence on the optical properties of a single self-assembled QD. From excitation-power dependent measurements, we find a long Auger recombination time of about 500 ns and a quenching of the trion transition by about 80 percent. Furthermore, we observe a broadening of the trion transition linewidth by up to a factor of two. With a model based on rate equations, we are able to identify the interplay between tunneling and Auger rate as the underlying mechanism for the reduced intensity and the broadening of the linewidth. This demonstrates that self-assembled QDs can serve as an ideal model system to study how the charge recapture process, given by the band-structure surrounding the confined carriers, influences the Auger process. Our findings are not only relevant for improving the emission properties of colloidal QD-based emitters and dyes, which have recently entered the consumer market. They are also of interest for more visionary applications, such as quantum information technologies, based on self-assembled quantum dots.

We study the optical response of a suspended graphene field-effect transistor in magnetic fields of up to 9 T (quantum Hall regime). With an illumination power of only 3 {\mu}W, we measure a photocurrent of up to 400 nA, corresponding to a photo-responsivity of 0.14 A/W, which we believe to be the highest value ever measured in single-layer graphene. We estimate that every absorbed photon creates more than 8 electron-hole pairs, which demonstrates highly effective carrier multiplication. As suggested by the dependence of the photocurrent on gate voltage and magnetic field, we propose a ballistic two-stage mechanism where the incident photons create primary charge carriers which then excite secondary charge carriers in the chiral edge states via Auger-type inelastic Coulomb scattering processes at the graphene edge., Comment: 11 Pages, 4 Figures

Using time-resolved transconductance spectroscopy, we study the tunneling dynamics between a two-dimensional electron gas (2DEG) and self-assembled quantum dots (QDs), embedded in a field-effect transistor structure. We find that the tunneling of electrons from the 2DEG into the QDs is governed by a different time constant than the reverse process, i.e., tunneling from the QDs to the 2DEG. This asymmetry is a clear signature of Coulomb interaction and makes it possible to determine the degeneracy of the quantum dot orbitals even when the individual states cannot be resolved energetically because of inhomogeneous broadening. Our experimental data can be qualitatively explained within a master-equation approach.