arXiv subjects

Arzhang Ardavan

Publications and source records attributed to Arzhang Ardavan.

At least 19 recordsLinked to original sources

arXiv2026

All-electrical Coherent Control of a Single Rare-earth Spin Qubit

Electrical control of single spin qubits is a major frontier for nanoscale, high-speed, and scalable quantum devices. Yet, extending it to highly shielded rare-earth 4f electrons remains an experimental challenge across solid-state platforms. Here we demonstrate all-electrical coherent control of a single Er electron spin, which is exchange-coupled to a nearby Ti atom. Scanning tunneling microscopy-based electron spin resonance with three-dimensional magnetic-field control enables comprehensive mapping of the resonance and Rabi frequencies, revealing pronounced anisotropies in both the Er g-tensor and the Er-Ti exchange interaction. The electrical modulation of the anisotropic Er-Ti coupling results in an efficient drive of the Er spin, allowing us to achieve near-gigahertz Rabi frequencies - a ten-fold improvement over the present record for rare-earth spin qubits. By establishing anisotropic exchange as a general resource for electrically accessing shielded rare-earth spins, our results open a new route to ultrafast and local control of rare-earth spins in solid-state quantum devices.

cond-mat.mes-hall↗

arXiv2026

Coherent electric field manipulation of nuclear spin qudit

Spins in condensed matter, especially well-isolated nuclear spins, offer attractive quantum degrees of freedom for computing, sensing, and networking because of their long coherence times. The possibility of electric-field control is an important feature for practical scalable quantum technologies, but, typically, nuclear spins couple only weakly to electric fields in conventional semiconductor hosts, limiting operation efficiency. Here we show that a choice of a highly polarizable oxide host can overcome this bottleneck. In Mn2+ doped ZnO, electric-field modulation of the spin Hamiltonian is amplified by hyperfine-coupled electron spins, and offers efficient electric-field manipulation of an I = 5/2 nuclear spin qudit, in a manner analogous to the hyperfine enhancement of conventional nuclear magnetic resonance. We demonstrate both resonant and non-resonant coherent manipulation using a single uniaxial electric field applied along the crystalline c-axis, the polarization axis of ZnO. This approach allows universal single-qudit gate operations with efficiencies comparable to or exceeding those of conventional magnetic-field driving. These results support the deployment of doped oxides as active host materials for electrically controllable spin qubits, highlighting the importance of materials design in developing scalable quantum technologies.

quant-ph↗

arXiv2025

Electric-field Quantum Sensing Exploiting a Photogenerated Charge-transfer Triplet State in a Molecular Semiconductor

Molecular spin systems are promising platforms for quantum sensing due to their chemically tunable Hamiltonians, enabling tailored coherence properties and interactions with external fields. However, electric field sensing remains challenging owing to typically weak spin-electric coupling (SEC) and limited directional sensitivity. Addressing these issues using heavy atoms exhibiting strong atomic spin-orbit couplings (SOC) often compromises spin coherence times. Here, we demonstrate coherent electric field sensing using a photogenerated charge-transfer (CT) spin triplet state in the organic molecule ACRSA (10-phenyl-10H,10' H-spiro\[acridine-9,9'-anthracen]-10'-one). By embedding electric field pulses within a Hahn echo sequence, we coherently manipulate the spin triplet and extract both the magnitude and directional dependence of its SEC. The measured SEC strength is approximately 0.51 Hz/(V/m), comparable to values reported in systems with strong atomic SOC, illustrating that heavy atoms are not a prerequisite for electric-field sensitivity of spin states. Our findings position organic CT triplets as chemically versatile and directionally sensitive quantum sensors of E-fields that function without atomic-SOC-mediated mechanisms.

quant-ph↗

arXiv2025

Programmable self-assembly for scalable molecular electronic architectures

Molecular electronics and other technologies whose components comprise individual molecules have been pursued for half a century because the molecular scale represents the limit of miniaturisation of objects whose structure is tuneable for function. Despite the promise, practical progress has been hindered by the lack of methodologies for directed assembly of arbitrary structures applicable at the molecular scale. DNA nanotechnology is an emerging framework that uses programmed synthetic oligomers to encode the design of self-assembling structures with atomic precision at the nanoscale. Here, we leverage DNA-directed self-assembly to construct single-molecule electrical transport devices in high yield, precisely positioning a metal-porphyrin between two 60 nm gold nanoparticles. Following deposition on SiO2 substrates, we image and establish electrical contact via established nanofabrication techniques. Each step of the process has a high success rate and we demonstrate device yields dramatically better than is possible using conventional approaches. Our approach is inherently scalable and adaptable to devices incorporating multiple heterogenous functional molecular components, finally offering a realistic framework for the realisation of classical and quantum molecular technologies.

cond-mat.mes-hall↗

arXiv2025

Designing quantum error correction codes for practical spin qudit

The implementation of practical error correction protocols is essential for deployment of quantum information technologies. Ways of exploiting high-spin nuclei, which have multi-level quantum resources, have attracted interest in this context because they offer additional Hilbert space dimensions in a spatially compact and theoretically efficient structure. We present a quantitative analysis of the performance of a spin-qudit-based error-correctable quantum memory, with reference to the actual Hamiltonians of several potential candidate systems. First, the ideal code-word implemented on a spin-7/2 nucleus, which provides first order Pauli-$X$, $Y$ and $Z$ error correction, has intrinsic infidelity due to mixed eigenstates under realistic conditions. We confirm that expansion to a spin-9/2 system with tailored code-words can compensate this infidelity. Second, we claim that electric field fluctuations -- which are inevitable in real systems -- should also be considered as a noise source, and we illustrate an encoding/decoding scheme for a multi-spin-qudit-based error correction code that can simultaneously compensate for both electric and magnetic field perturbations. Such strategies are important as we move beyond the current noisy-intermediate quantum era, and fidelities above two or three nines becomes crucial for implementation of quantum technologies.

quant-ph↗

arXiv2025

Demonstrating experimentally the encoding and dynamics of an error-correctable logical qubit on a hyperfine-coupled nuclear spin qudit

The realization of effective quantum error correction protocols remains a central challenge in the development of scalable quantum computers. Employing high-dimensional quantum systems (qudits) can offer more hardware-efficient protocols than qubit-based approaches. Using electron-nuclear double resonance, we implement a logical qubit encoded on the four states of a I=3/2 nuclear spin hyperfine-coupled to a S=1/2 electron spin qubit; the encoding protects against the dominant decoherence mechanism in such systems, fluctuations of the quantizing magnetic field. We explore the dynamics of the encoded state both under a controlled application of the fluctuation and under natural decoherence processes. Our results confirm the potential of these proposals for practical, implementable, fault tolerant quantum memories.

quant-ph↗

arXiv2024

Chemical tuning of quantum spin-electric coupling in molecular nanomagnets

Controlling quantum spins using electric rather than magnetic fields promises significant architectural advantages for developing quantum technologies. In this context, spins in molecular nanomagnets offer tunability of spin-electric couplings (SEC) by rational chemical design. Here we demonstrate systematic control of SECs in a family of Mn(II)-containing molecules via chemical engineering. The trigonal bipyramidal (tbp) molecular structure with C3 symmetry leads to a significant molecular electric dipole moment that is directly connected to its magnetic anisotropy. The interplay between these two features gives rise to significant experimentally observed SECs, which can be rationalised by wavefunction theoretical calculations. Our findings guide strategies for the development of electrically controllable molecular spin qubits for quantum technologies.

cond-mat.mes-hall↗

arXiv2024

A continuous-wave and pulsed X-band electron spin resonance spectrometer operating in ultra-high vacuum for the study of low dimensional spin ensembles

We report the development of a continuous-wave and pulsed X-band electron spin resonance (ESR) spectrometer for the study of spins on ordered surfaces down to cryogenic temperatures. The spectrometer operates in ultra-high vacuum and utilizes a half-wavelength microstrip line resonator realized using epitaxially grown copper films on single crystal Al$_2$O$_3$ substrates. The one-dimensional microstrip line resonator exhibits a quality factor of more than 200 at room temperature, close to the upper limit determined by radiation losses. The surface characterizations of the copper strip of the resonator by atomic force microscope, low-energy electron diffraction, and scanning tunneling microscope show that the surface is atomically clean, flat, and single crystalline. Measuring the ESR spectrum at 15 K from a few nm thick molecular film of YPc$_2$, we find a continuous-wave ESR sensitivity of $2.6 \cdot 10^{11}~\text{spins}/\text{G} \cdot \text{Hz}^{1/2}$ indicating that a signal-to-noise ratio of $3.9~\text{G} \cdot \text{Hz}^{1/2}$ is expected from a monolayer of YPc$_2$ molecules. Advanced pulsed ESR experimental capabilities including dynamical decoupling and electron-nuclear double resonance are demonstrated using free radicals diluted in a glassy matrix.

cond-mat.mes-hall↗

arXiv2024

High-field immiscibility of electrons belonging to adjacent twinned bismuth crystals

Bulk bismuth has a complex Landau spectrum. The small effective masses and the large g-factors are anisotropic. The chemical potential drifts at high magnetic fields. Moreover, twin boundaries further complexify the interpretation of the data by producing extra anomalies in the extreme quantum limit. Here, we present a study of angle dependence of magnetoresistance up to 65 T in bismuth complemented with Nernst, ultrasound, and magneto-optic data. All observed anomalies can be explained in a single-particle picture of a sample consisting of two twinned crystals tilted by 108$^{\circ}$ and with two adjacent crystals keeping their own chemical potentials despite a shift between chemical potentials as large as 68 meV at 65 T. This implies an energy barrier between adjacent twinned crystals reminiscent of a metal-semiconductor Schottky barrier or a p-n junction. We argue that this barrier is built by accumulating charge carriers of opposite signs across a twin boundary.

cond-mat.mtrl-sci↗

arXiv2024

All-electrical driving and probing of dressed states in a single spin

The sub-nanometer distance between tip and sample in a scanning tunneling microscope (STM) enables the application of very large electric fields with a strength as high as ~ 1 GV/m. This has allowed for efficient electrical driving of Rabi oscillations of a single spin on a surface at a moderate radio-frequency (RF) voltage of the order of tens of millivolts. Here, we demonstrate the creation of dressed states of a single electron spin localized in the STM tunnel junction by using resonant RF driving voltages. The read-out of these dressed states was achieved all-electrical by a weakly coupled probe spin. Our work highlights the strength of the atomic-scale geometry inherent to the STM that facilitates creation and control of dressed states, which are promising for a design of atomically well-defined single spin quantum devices on surfaces.

cond-mat.mes-hall↗

arXiv2023

Fault-tolerant qubit encoding using a spin-7/2 qudit

The implementation of error correction protocols is a central challenge in the development of practical quantum information technologies. Recently, multi-level quantum resources such as harmonic oscillators and qudits have attracted interest in this context because they offer the possibility of additional Hilbert space dimensions in a spatially compact way. Here we propose a quantum memory, implemented on a spin-7/2 nucleus hyperfine-coupled to an electron spin-1/2 qubit, which provides first order $X$, $Y$ and $Z$ error correction using significantly fewer quantum resources than the equivalently effective qubit-based protocols. Our encoding may be efficiently implemented in existing experimentally realised molecular electron-nuclear quantum spin systems. The strategy can be extended to higher-order error protection on higher-spin nuclei.

quant-ph↗

arXiv2022

Quantum-Coherent Nanoscience

For the past three decades, nanoscience has widely affected many areas in physics, chemistry, and engineering, and has led to numerous fundamental discoveries as well as applications and products. Concurrently, quantum science and technology has developed into a cross-disciplinary research endeavour connecting these same areas and holds a burgeoning commercial promise. Although quantum physics dictates the behaviour of nanoscale objects, quantum coherence, which is central to quantum information, communication and sensing has not played an explicit role in much of nanoscience. This Review describes fundamental principles and practical applications of quantum coherence in nanoscale systems, a research area we call quantum-coherent nanoscience. We structure this manuscript according to specific degrees of freedom that can be quantum-coherently controlled in a given nanoscale system such as charge, spin, mechanical motion, and photons. We review the current state of the art and focus on outstanding challenges and opportunities unlocked by the merging of nanoscience and coherent quantum operations.

cond-mat.mes-hall↗

arXiv2021

Superconducting fluctuations observed far above T$_\mathrm{c}$ in the isotropic superconductor K$_3$C$_{60}$

Alkali-doped fullerides are strongly correlated organic superconductors that exhibit high transition temperatures, exceptionally large critical magnetic fields and a number of other unusual properties. The proximity to a Mott insulating phase is thought to be a crucial ingredient of the underlying physics, and may also affect precursors of superconductivity in the normal state above T$_\text{c}$. We report on the observation of a sizeable magneto-thermoelectric (Nernst) effect in the normal state of K$_3$C$_{60}$, which displays the characteristics of superconducting fluctuations. The anomalous Nernst effect emerges from an ordinary quasiparticle background below a temperature of 80K, far above T$_\text{c}$ = 20K. At the lowest fields and close to T$_\text{c}$, the scaling of the effect is captured by a model based on Gaussian fluctuations. The temperature up to which we observe fluctuations is exceptionally high for a three-dimensional isotropic system, where fluctuation effects are usually suppressed.

cond-mat.supr-con↗

arXiv2021

Quantum coherent spin-electric control in a molecular nanomagnet at clock transitions

Electrical control of spins at the nanoscale offers significant architectural advantages in spintronics, because electric fields can be confined over shorter length scales than magnetic fields. Thus, recent demonstrations of electric-field (E-field) sensitivities in molecular spin materials are tantalising, raising the viability of the quantum analogues of macroscopic magneto-electric devices.However, the E-field sensitivities reported so far are rather weak, prompting the question of how to design molecules with stronger spin-electric couplings. Here we show that one path is to identify an energy scale in the spin spectrum that is associated with a structural degree of freedom with a significant electrical polarisability. We study an example of a molecular nanomagnet in which a small structural distortion establishes clock transitions (i.e. transitions whose energy is to first order independent of magnetic field) in the spin spectrum; the fact that this distortion is associated with an electric dipole allows us to control the clock transition energy to an unprecedented degree. We demonstrate coherent electrical control of the quantum spin state and exploit it to manipulate independently the two magnetically-identical but inversion-related molecules in the unit cell of the crystal. Our findings pave the way for the use of molecular spins in quantum technologies and spintronics.

cond-mat.mes-hall↗

arXiv2020

Universal limiting transition temperature for the high $T_\mathrm{c}$ superconductors

Since their discovery three decades ago it has emerged that the physics of high-$T_\mathrm{c}$ cuprate superconductors is characterised by multiple temperature scales, and a phenomenology that deviates significantly from the conventional paradigm of superconductivity. Below the "pseudogap" temperature, $T^*$, a range of experiments indicate a reduction in the density of states. Lower in temperature, $T_\mathrm{c}$ marks the onset of a bulk zero-resistance state. Intermediate between these, numerous other temperature boundaries and cross-overs have been identified, often postulated to be associated with fluctuations of some kind. However, for the most part there is little consensus either over their definitions or the physical mechanisms at play. One of these temperature scales is the Nernst onset temperature, $T_\mathrm{onset}$, below which thermoelectric phenomena characteristic of superconductivity are observed. Depending on the material, the difference between $T_\mathrm{onset}$ and $T_\mathrm{c}$ ranges from almost nothing to over 100K. In this paper, we identify $T_\mathrm{onset}$ from published experimental data according to a consistent definition; this reveals a remarkable consistency of behaviour across the whole high-$T_\mathrm{c}$ family, despite the appreciable variations in other parameters. Our analysis suggests that in the cuprates there is an inherent limit to $T_\mathrm{c} \sim 135$K. We compare this behaviour with other strongly-correlated superconductors and propose a unified picture of superconducting fluctuations close to the Mott state.

cond-mat.supr-con↗

arXiv2019

Mott polaritons in cavity-coupled quantum materials

We show that strong electron-electron interactions in cavity-coupled quantum materials can enable collectively enhanced light-matter interactions with ultrastrong effective coupling strengths. As a paradigmatic example we consider a Fermi-Hubbard model coupled to a single-mode cavity and find that resonant electron-cavity interactions result in the formation of a quasi-continuum of polariton branches. The vacuum Rabi splitting of the two outermost branches is collectively enhanced and scales with $g_{\text{eff}}\propto\sqrt{2L}$, where $L$ is the number of electronic sites, and the maximal achievable value for $g_{\text{eff}}$ is determined by the volume of the unit cell of the crystal. We find that $g_{\text{eff}}$ for existing quantum materials can by far exceed the width of the first excited Hubbard band. This effect can be experimentally observed via measurements of the optical conductivity and does not require ultra-strong coupling on the single-electron level. Quantum correlations in the electronic ground state as well as the microscopic nature of the light-matter interaction enhance the collective light-matter interaction compared to an ensemble of independent two-level atoms interacting with a cavity mode.

cond-mat.str-el↗

arXiv2019

Manipulating quantum materials with quantum light

We show that the macroscopic magnetic and electronic properties of strongly correlated electron systems can be manipulated by coupling them to a cavity mode. As a paradigmatic example we consider the Fermi-Hubbard model and find that the electron-cavity coupling enhances the magnetic interaction between the electron spins in the ground-state manifold. At half filling this effect can be observed by a change in the magnetic susceptibility. At less than half filling, the cavity introduces a next-nearest neighbour hopping and mediates a long-range electron-electron interaction between distant sites. We study the ground state properties with Tensor Network methods and find that the cavity coupling can induce a new phase characterized by a momentum-space pairing effect for electrons.

cond-mat.str-el↗

arXiv2018

Electric field control of spins in molecular magnets

Coherent control of individual molecular spins in nano-devices is a pivotal prerequisite for fulfilling the potential promised by molecular spintronics. By applying electric field pulses during time-resolved electron spin resonance measurements, we measure the sensitivity of the spin in several antiferromagnetic molecular nanomagnets to external electric fields. We find a linear electric field dependence of the spin states in Cr$_7$Mn, an antiferromagnetic ring with a ground-state spin of $S=1$, and in a frustrated Cu$_3$ triangle, both with coefficients of about $2~\mathrm{rad}\, \mathrm{s}^{-1} / \mathrm{V} \mathrm{m}^{-1}$. Conversely, the antiferromagnetic ring Cr$_7$Ni, isomorphic with Cr$_7$Mn but with $S=1/2$, does not exhibit a detectable effect. We propose that the spin-electric field coupling may be used for selectively controlling individual molecules embedded in nanodevices.

cond-mat.str-el↗