Huma Yusuf, Michael Chilcote, Denis R. Candido, Seth W. Kurfman, Donley S. Cormode, Yu Lu, Michael E. Flatté, Ezekiel Johnston-Halperin
Quantum information science and engineering requires novel low-loss magnetic materials for magnon-based quantum-coherent operations. The search for low-loss magnetic materials, traditionally driven by applications in microwave electronics near room-temperature, has gained additional constraints from the need to operate at cryogenic temperatures for many applications in quantum information science and technology. Whereas yttrium iron garnet (YIG) has been the material of choice for decades, the emergence of molecule-based materials with robust magnetism and ultra-low damping has opened new avenues for exploration. Specifically, thin-films of vanadium tetracyanoethylene (V[TCNE]x) can be patterned into the multiple, connected structures needed for hybrid quantum elements and have shown room-temperature Gilbert damping (α = 4 \times 10^-5) that rivals the intrinsic (bulk) damping otherwise seen only in highly-polished YIG spheres (far more challenging to integrate into arrays). Here, we present a comprehensive and systematic study of the low-temperature magnetization dynamics for V[TCNE]x thin films, with implications for their application in quantum systems. These studies reveal a temperature-driven, strain-dependent magnetic anisotropy that compensates the thin-film shape anisotropy, and the recovery of a magnetic resonance linewidth at 5 K that is comparable to room-temperature values (roughly 2 G at 9.4 GHz). We can account for these variations of the V[TCNE]x linewidth within the context of scattering from very dilute paramagnetic impurities, and anticipate additional linewidth narrowing as the temperature is further reduced.
Warlley H. Campos, Poliana H. Penteado, Julian Zanon, Paulo E. Faria Junior, Denis R. Candido, J. Carlos Egues
Dual topological insulators (DTIs) are simultaneously protected by time-reversal and crystal symmetries, representing advantageous alternatives to conventional topological insulators. By combining ab initio calculations and the $\mathbf{k}\cdot\mathbf{p}$ approach, here, we investigate the electronic band structure of a Na$_2$CdSn triatomic layer and derive a low-energy $4\times 4$ effective model consistent with all the symmetries of this material class. We obtain the effective Hamiltonian using the Löwdin perturbation theory, the folding-down technique, and the theory of invariants and determine its parameters by fitting our analytical dispersion relations to those of ab initio calculations. We then calculate the bulk topological invariants of the system and show that the Na$_2$CdSn triatomic layer is a giant-gap (hundreds of millielectronvolts) quasi-two-dimensional DTI characterized by both spin and mirror Chern numbers $-2$. In agreement with the bulk-boundary correspondence theorem, we find that a finite-width strip of Na$_2$CdSn possesses two pairs of counterpropagating helical edge states per interface. We obtain analytical expressions for the edge state energy dispersions and wave functions, which are shown to agree with our numerical calculations. Our work opens an avenue for further studies of Na$_2$CdSn as a potential DTI candidate with room-temperature applications in areas of technological interest, such as nanoelectronics and spintronics.
Hamed Gramizadeh, Denis R. Candido, Andrei Manolescu, J. Carlos Egues, Sigurdur I. Erlingsson
Magneto-oscillations in two-dimensional systems with spin-orbit interaction are typically characterized by fast Shubnikov-de~Haas (SdH) oscillations and slower spin-orbit-related beatings. The characterization of the full SdH oscillatory behavior in systems with both spin-orbit interaction and Zeeman coupling requires a time consuming diagonalization of large matrices for many magnetic field values. By using the Poisson summation formula we can explicitly separate the density of states into, fast and slow oscillations, which determine the corresponding fast and slow parts of the magneto-oscillations. We introduce an efficient scheme of partial diagonalization of our Hamiltonian, where only states close to the Fermi energy are needed to obtain the SdH oscillations, thus reducing the required computational time. This allows an efficient method for fitting numerically the SdH data, using the inherent separation of the fast and slow oscillations. We compare systems with only Rashba spin-orbit interaction (SOI) and both Rashba and Dresselhaus SOI with, and without, an in-plane magnetic field. The energy spectra are characterized in terms of symmetries, which have direct and visible consequences in the magneto-oscillations. To highlight the benefits of our methodology, we use it to extract the spin-orbit parameters by fitting realistic transport data.
Uri Zvi, Shivam Mundhra, David Ovetsky, Qing Chen, Aidan R. Jones, Stella Wang, Maria Roman, Michele Ferro, Kunle Odunsi, Marina C. Garassino, Michael E. Flatte', Melody Swartz, Denis R. Candido, Aaron Esser-Kahn, Peter C. Maurer
Nitrogen-vacancy (NV) based quantum sensors hold great potential for real-time single-cell sensing with far-reaching applications in fundamental biology and medical diagnostics. Although highly sensitive, the mapping of quantum measurements onto cellular physiological states has remained an exceptional challenge. Here we introduce a novel quantum sensing modality capable of detecting changes in cellular activity. Our approach is based on the detection of environment-induced charge depletion within an individual particle that, owing to a previously unaccounted transverse dipole term, induces systematic shifts in the zero-field splitting (ZFS). Importantly, these charge-induced shifts serve as a reliable indicator for lipopolysaccharide (LPS)-mediated inflammatory response in macrophages. Furthermore, we demonstrate that surface modification of our diamond nanoprobes effectively suppresses these environment-induced ZFS shifts, providing an important tool for differentiating electrostatic shifts caused by the environment from other unrelated effects, such as temperature variations. Notably, this surface modification also leads to significant reductions in particle-induced toxicity and inflammation. Our findings shed light on systematic drifts and sensitivity limits of NV spectroscopy in a biological environment with ramification on the critical discussion surrounding single-cell thermogenesis. Notably, this work establishes the foundation for a novel sensing modality capable of probing complex cellular processes through straightforward physical measurements.
Yogendra Limbu, Hari Paudyal, Eudes Gomes da Silva, Denis R. Candido, Michael E. Flatté, Durga Paudyal
We report an \textit{ab initio} investigation of functionalized and 3$d$-electrons doped Cr$_2$C MXenes. Upon functionalization, the Cr$_2$C becomes chemically, dynamically, and mechanically stable, and it exhibits magnetic semiconducting behavior. Cr$_2$CF$_2$ stands out as a wide band gap semiconductor, possessing super exchange interaction mediated by F atoms within the layer, however, the applied strain transforms it from an indirect to a direct band gap semiconductor. Strong spin-phonon coupling found in Cr$_2$CH$_2$ is supported by the distorted Cr spin density due to hydrogen environment. Two magnon branches, associated with two sub-lattice spins, are found in the ferromagnetic Cr$_2$CO$_2$ and antiferromagnetic Cr$_2$CF$_2$. Depending on the types of 3$d$-electron dopants and functionalization, Cr$_2$C MXenes (except for Cr$_2$CO$_2$) change from the indirect band gap magnetic semiconductor to different states of electronic and magnetic matter including exotic direct band gap magnetic bipolar semiconductor. In addition, we reveal a band inversion between the two highest valence bands in the Fe-doped Cr$_2$CCl$_2$.
Masaya Fukami, Jonathan C. Marcks, Denis R. Candido, Leah R. Weiss, Benjamin Soloway, Sean E. Sullivan, Nazar Delegan, F. Joseph Heremans, Michael E. Flatté, David D. Awschalom
Aug 22, 2023·quant-ph·PDF Controlled interaction between localized and delocalized solid-state spin systems offers a compelling platform for on-chip quantum information processing with quantum spintronics. Hybrid quantum systems (HQSs) of localized nitrogen-vacancy (NV) centers in diamond and delocalized magnon modes in ferrimagnets-systems with naturally commensurate energies-have recently attracted significant attention, especially for interconnecting isolated spin qubits at length-scales far beyond those set by the dipolar coupling. However, despite extensive theoretical efforts, there is a lack of experimental characterization of the magnon-mediated interaction between NV centers, which is necessary to develop such hybrid quantum architectures. Here, we experimentally determine the magnon-mediated NV-NV coupling from the magnon-induced self-energy of NV centers. Our results are quantitatively consistent with a model in which the NV center is coupled to magnons by dipolar interactions. This work provides a versatile tool to characterize HQSs in the absence of strong coupling, informing future efforts to engineer entangled solid-state systems.
Seth W. Kurfman, Denis R. Candido, Brandi Wooten, Yuanhua Zheng, Michael J. Newburger, Shuyu Cheng, Roland K. Kawakami, Joseph P. Heremans, Michael E. Flatté, Ezekiel Johnston-Halperin
Spintronic, spin caloritronic, and magnonic phenomena arise from complex interactions between charge, spin, and structural degrees of freedom that are challenging to model and even more difficult to predict. This situation is compounded by the relative scarcity of magnetically-ordered materials with relevant functionality, leaving the field strongly constrained to work with a handful of well-studied systems that do not encompass the full phase space of phenomenology predicted by fundamental theory. Here we present an important advance in this coupled theory-experiment challenge, wherein we extend existing theories of the spin Seebeck effect (SSE) to explicitly include the temperature-dependence of magnon non-conserving processes. This expanded theory quantitatively describes the low-temperature behavior of SSE signals previously measured in the mainstay material yttrium iron garnet (YIG) and predicts a new regime for magnonic and spintronic materials that have low saturation magnetization, $M_S$, and ultra-low damping. Finally, we validate this prediction by directly observing the spin Seebeck resistance (SSR) in the molecule-based ferrimagnetic semiconductor vanadium tetracyanoethylene (V[TCNE]$_x$, $x \sim 2$). These results validate the expanded theory, yielding SSR signals comparable in magnitude to YIG and extracted magnon diffusion length ($λ_m>1$ $μ$ m) and magnon lifetime for V[TCNE]$_x$ ($τ_{th}\approx 1-10$ $μ$ s) exceeding YIG ($τ_{th}\sim 10$ ns). Surprisingly, these properties persist to room temperature despite relatively low spin wave stiffness (exchange). This identification of a new regime for highly efficient SSE-active materials opens the door to a new class of magnetic materials for spintronic and magnonic applications.
Henry C. Hammer, Hassan A. Bukhari, Yogendra Limbu, Brett M. Wasick, Christopher Rouleau, Michael E. Flatté, Durga Paudyal, Denis R. Candido, Ravitej Uppu
Nov 24, 2025·quant-ph·PDF Harnessing rare-earth ions in oxides for quantum networks requires integration with bright emitters in III-V semiconductors, but local disorder and interfacial noise limit their optical coherence. Here, we investigate the microscopic origins of the ensemble spectrum in Er$^{3+}$:TiO$_2$ epitaxial thin films on GaAs and GaSb substrates. Ab initio calculations combined with noise-Hamiltonian modeling and Monte Carlo simulations quantify the effects of interfacial and bulk spin noise and local strain on erbium crystal-field energies and inhomogeneous linewidths. Photoluminescence excitation spectroscopy reveals that Er$^{3+}$ ions positioned at increasing distances from the III-V/oxide interface produce a systematic blue shift of the $Y_1\rightarrow Z_1$ transition, consistent with strain relaxation predicted by theory. Thermal annealing produces a compensating redshift and linewidth narrowing, isolating the roles of oxygen-vacancy and gallium-diffusion noise. These results provide microscopic insight into disorder-driven decoherence, offering pathways for precise control of hybrid quantum systems for scalable quantum technologies.
Xiaofei Yu, Evan J. Villafranca, Stella Wang, Jessica C. Jones, Mouzhe Xie, Jonah Nagura, Ignacio Chi-Durán, Nazar Delegan, Alex B. F. Martinson, Michael E. Flatté, Denis R. Candido, Giulia Galli, Peter C. Maurer
Apr 11, 2025·quant-ph·PDF Nitrogen-vacancy (NV) centers in diamond are extensively utilized as quantum sensors for imaging fields at the nanoscale. The ultra-high sensitivity of NV magnetometers has enabled the detection and spectroscopy of individual electron spins, with potentially far-reaching applications in condensed matter physics, spintronics, and molecular biology. However, the surfaces of these diamond sensors naturally contain electron spins, which create a background signal that can be hard to differentiate from the signal of the target spins. In this study, we develop a surface modification approach that eliminates the unwanted signal of these so-called dark electron spins. Our surface passivation technique, based on coating diamond surfaces with a thin titanium oxide (TiO$_2$) layer, reduces the dark spin density. The observed reduction in dark spin density aligns with our findings on the electronic structure of the diamond-TiO$_2$ interface. The reduction, from a typical value of $2,000$~$μ$m$^{-2}$ to a value below that set by the detection limit of our NV sensors ($200$~$μ$m$^{-2}$), results in a two-fold increase in Hahn-echo coherence time of near surface NV centers. Furthermore, we derive a comprehensive spin model that connects dark spin relaxation with NV coherence, providing additional insights into the mechanisms behind the observed spin dynamics. Our findings are directly transferable to other quantum platforms, including nanoscale solid state qubits and superconducting qubits.
Denis R. Candido, Maxim Kharitonov, J. Carlos Egues, Ewelina M. Hankiewicz
We present a paradoxical finding that, in the vicinity of a topological phase transition in a quantum anomalous Hall system (Chern insulator), topology nearly always (except when the system obeys charge-conjugation symmetry) results in a significant extension of the edge-state structure beyond the minimal one required to satisfy the Chern numbers. The effect arises from the universal gapless linear-in-momentum Hamiltonian of the nodal semimetal describing the system right at the phase transition, whose form is enforced by the change of the Chern number. Its emergent approximate chiral symmetry results in an edge-state band in the vicinity of the node, in the region of momenta where such form is dominant. Upon opening the gap, this edge-state band is modified in the gap region, becoming "protected" (connected to the valence bulk band with one end and conduction band with the other) in the topologically nontrivial phase and "nonprotected" (connected to either the valence or conduction band with both ends) in the trivial phase. The edge-state band persists in the latter as long as the gap is small enough.
Antonio Zegarra, Denis R. Candido, J. Carlos Egues, Wei Chen
We present a Green's function formalism to investigate the topological properties of weakly interacting one-dimensional topological insulators, including the bulk-edge correspondence and the quantum criticality near topological phase transitions, and using interacting Su-Schrieffer-Heeger model as an example. From the many-body spectral function, we find that closing of the bulk gap remains a defining feature even if the topological phase transition is driven by interactions. The existence of edge state in the presence of interactions can be captured by means of a T-matrix formalism combined with Dyson's equation, and the bulk-edge correspondence is shown to be satisfied even in the presence of interactions. The critical exponent of the edge state decay length is shown to be affiliated with the same universality class as the noninteracting limit.
Denis R. Candido, Michael E. Flatté
Mar 23, 2023·quant-ph·PDF Decoherence and relaxation of solid-state defect qutrits near a crystal surface, where they are commonly used as quantum sensors, originates from charge and magnetic field noise. A complete theory requires a formalism for decoherence and relaxation that includes all Hamiltonian terms allowed by the defect's point-group symmetry. This formalism, presented here for the $C_{3v}$ symmetry of a spin-1 defect in a diamond, silicon cardide, or similar host, relies on a Lindblad dynamical equation and clarifies the relative contributions of charge and spin noise to relaxation and decoherence, along with their dependence on the defect spin's depth and resonant frequencies. The calculations agree with the experimental measurements of Sangtawesin $\textit{et al.}$, Phys. Rev. X $\textbf{9}$, 031052 (2019) and point to an unexpected importance of charge noise.
Uri Zvi, Denis R. Candido, Adam Weiss, Aidan R. Jones, Lingjie Chen, Iryna Golovina, Xiaofei Yu, Stella Wang, Dmitri V. Talapin, Michael E. Flatté, Aaron P. Esser-Kahn, Peter C. Maurer
Diamond nanocrystals can harbor spin qubit sensors capable of probing the physical properties of biological systems with nanoscale spatial resolution. These diamond nanosensors can readily be delivered into intact cells and even living organisms. However, applications beyond current proof-of-principle experiments require a substantial increase in sensitivity, which is generally limited by surface-noise-induced spin dephasing and relaxation. In this work, we significantly reduce magnetic surface noise by engineering core-shell structures, which in combination with dynamical decoupling result in qubit coherence times (T2) ranging from 52us to 87us - a drastic improvement over the 1.1us to 35us seen in bare particles. This improvement in spin coherence, combined with an overall increase in particle fluorescence, corresponds to a two-order-of-magnitude reduction in integration time. Probing qubit dynamics at a single particle level, furthermore, reveals that the noise characteristics fundamentally change from a bath with spins that rearrange their spatial configuration during the course of an experiment to a more dilute static bath. The observed results shed light on the underlying mechanisms governing spin dephasing in diamond nanocrystals and offer an effective noise mitigation strategy based on engineered core-shell structures.
Denis R. Candido, Sigurdur I. Erlingsson, João Vitor I. Costa, J. Carlos Egues
We investigate the Shubnikov-de Haas (SdH) magneto-oscillations in the resistivity of two-dimensional topological insulators (TIs). Within the Bernevig-Hughes-Zhang (BHZ) model for TIs in the presence of a quantizing magnetic field, we obtain analytical expressions for the SdH oscillations by combining a semiclassical approach for the resistivity and a trace formula for the density of states. We show that when the non-trivial topology is produced by inverted bands with ''Mexican-hat'' shape, SdH oscillations show an anomalous beating pattern that is {\it solely} due to the non-trivial topology of the system. These beatings are robust against, and distinct from beatings originating from spin-orbit interactions. This provides a direct way to experimentally probe the non-trivial topology of 2D TIs entirely from a bulk measurement. Furthermore, the Fourier transform of the SdH oscillations as a function of the Fermi energy and quantum capacitance models allows for extracting both the topological gap and gap at zero momentum.
Antônio C. Lourenço, Denis R. Candido, Eduardo I. Duzzioni
May 21, 2024·quant-ph·PDF Here, we calculate and study correlations of the Dicke model in the presence of qubit-qubit interaction. Whereas the analysis of correlations among its subsystems is essential for the understanding of corresponding critical phenomena and for performing quantum information tasks, the majority of correlation measures are restricted to bipartitions due to the inherent challenges associated with handling multiple partitions. To circunvent this we employ the calculation of Genuine Multipartite Correlations (GMC) based on the invariance of our model under particle permutation. We then quantify the correlations within each subpart of the system, as well as the percentage contribution of each GMC of order $k$, highlighting the many-body behaviors for different regimes of parameters. Additionally, we show that GMC signal both first- and second-order quantum phase transitions present in the model. Furthermore, as GMC encompasses both classical and quantum correlations, we employ Quantum Fisher Information (QFI) to detect genuine multipartite entanglement. Ultimately, we map the Dicke model with interacting qubits to spin in solids interacting with a quantum field of magnons, thus demonstrating a potential experimental realization of this model.
Denis R. Candido, Michael E. Flatté
Surface electric (charge) noise influences spin defects due to fluctuation of the surface charge density and also the electrostatic potential at the crystal surface. Surprisingly, the two-point correlation function of both the charged particles' positions and the surface electrostatic potential strongly influences the power of the polynomial decay of the electric noise spectral density; this power is not determined solely by the character of the charge fluctuators. Time-dependent crossover behavior near the correlation time of the fluctuators, of the spin defect's relaxation and decoherence, provide a quantitative fingerprint of the diffusive behavior of charged particles at the surface.
Troy Losey, Denis R. Candido, Jin Zhang, Y. Meurice, M. E. Flatté, S. -W. Tsai
In this work we propose a novel solid-state platform for creating quantum simulators based on implanted spin centers in semiconductors. We show that under the presence of an external magnetic field, an array of $S=1$ spin centers interacting through magnetic dipole-dipole interaction can be mapped into an effective spin-half system equivalent to the XYZ model in an external magnetic field. Interestingly, this system presents a wide range of quantum phases and critical behaviors that can be controlled via magnetic field and orientational arrangement of the spin centers. We demonstrate our interacting spin chain can be tuned to both isotropic Heisenberg model and transverse-field Ising universality class. Notably, our model contains a line where the system is in a critical floating phase that terminates at Berezinskii-Kosterlitz-Thouless and Pokrovsky-Talapov transition points. We propose this system as the first solid-state quantum simulator for the floating phase based on spin centers.
Denis R. Candido, Sigurdur I. Erlingsson, Hamed Gramizadeh, João Vitor I. Costa, Pirmin J. Weigele, Dominik M. Zumbühl, J. Carlos Egues
Shubnikov-de Haas (SdH) oscillations have served as a paradigmatic experimental probe and tool for extracting key semiconductor parameters such as carrier density, effective mass, Zeeman splitting with g-factor $g^*$, quantum scattering times and spin-orbit (SO) coupling parameters. Here, we derive for the first time an analytical formulation for the SdH oscillations in 2D electron gases (2DEGs) with simultaneous Rashba, Dresselhaus, and Zeeman interactions. Our analytical and numerical calculations allow us to extract both Rashba and Dresselhaus SO coupling parameters, carrier density, quantum lifetimes, and also to understand the role of higher harmonics in the SdH oscillations. More importantly, we derive a simple condition for the vanishing of SO induced SdH beatings for all harmonics in 2DEGs: $α/β= [(1-\tilde Δ)/(1+\tilde Δ)]^{1/2}$, where $\tilde Δ$ is a material parameter given by the ratio of the Zeeman and Landau level splitting. We also predict beatings in the higher harmonics of the SdH oscillations and elucidate the inequivalence of the SdH response of Rashba-dominated ($α>β$) vs Dresselhaus-dominated ($α<β$) 2DEGs in semiconductors with substantial $g^*$. We find excellent agreement with recent available experimental data of Dettwiler ${\it et\thinspace al.}$ Phys. Rev. X $\textbf{7}$, 031010 (2017), and Beukman ${\it et\thinspace al.}$, Phys. Rev. B $\textbf{96}$, 241401 (2017).
Jonatan A. Posligua, David E. Stewart, Denis R. Candido
Apr 23, 2026·quant-ph·PDF Solid-state spin defects hold great promise as building blocks for various quantum technologies. Embedding spin centers in $p$-$n$ diodes under reverse bias has proved to be a powerful strategy to narrow the optical linewidth and increase spin coherence, while also enabling control of the photoluminescence wavelength via Stark shift. Given the multitude of parameters influencing spin centers in diodes (e.g., doping densities and profiles, temperature, bias voltage, spin center position), a question that has not yet been answered is: which set of these design parameters maximizes spin center coherence? In this work, we address this question by developing a scaled gradient descent optimization algorithm that minimizes the optical linewidth of spin centers by combining the numerical solution of a diode's Poisson equation with calculated charge noise from the non-depleted regions. Our optimization is performed for both single- and multiple-parameter cases for divacancies in SiC $p$-$i$-$n$ diodes, including reverse-bias voltage, doping density and profile, and diode total length. Importantly, the optimization is subject to realistic physical constraints, such as small operating bias voltages, avoidance of the dielectric breakdown regime and physical thresholds for doping density. Additionally, due to the leakage current at reverse bias voltages, we develop a new formalism to investigate its influence on coherence. We show that the corresponding noise can be mitigated by implanting spin defects away from the diode's surfaces. Our work provides guidance on experimentally relevant diodes for hosting spin centers with the narrowest optical linewidths and longest coherence times.
Andrew Franson, Na Zhu, Seth Kurfman, Michael Chilcote, Denis R. Candido, Kristen S. Buchanan, Michael E. Flatté, Hong X. Tang, Ezekiel Johnston-Halperin
Integrating patterned, low-loss magnetic materials into microwave devices and circuits presents many challenges due to the specific conditions that are required to grow ferrite materials, driving the need for flip-chip and other indirect fabrication techniques. The low-loss ($α= 3.98 \pm 0.22 \times 10^{-5}$), room-temperature ferrimagnetic coordination compound vanadium tetracyanoethylene ($\mathrm{V[TCNE]}_x$) is a promising new material for these applications that is potentially compatible with semiconductor processing. Here we present the deposition, patterning, and characterization of $\mathrm{V[TCNE]}_x$ thin films with lateral dimensions ranging from 1 micron to several millimeters. We employ electron-beam lithography and liftoff using an aluminum encapsulated poly(methyl methacrylate), poly(methyl methacrylate-methacrylic acid) copolymer bilayer (PMMA/P(MMA-MAA)) on sapphire and silicon. This process can be trivially extended to other common semiconductor substrates. Films patterned via this method maintain low-loss characteristics down to 25 microns with only a factor of 2 increase down to 5 microns. A rich structure of thickness and radially confined spin-wave modes reveals the quality of the patterned films. Further fitting, simulation, and analytic analysis provides an exchange stiffness, $A_{ex} = 2.2 \pm 0.5 \times 10^{-10}$ erg/cm, as well as insights into the mode character and surface spin pinning. Below a micron, the deposition is non-conformal, which leads to interesting and potentially useful changes in morphology. This work establishes the versatility of $\mathrm{V[TCNE]}_x$ for applications requiring highly coherent magnetic excitations ranging from microwave communication to quantum information.