arXiv subjects

Chandrasekhar Ramanathan

Publications and source records attributed to Chandrasekhar Ramanathan.

At least 19 recordsLinked to original sources

arXiv2026

Optically detected nuclear magnetic resonance of carbon-13 in bulk diamond

Precision measurements based on optically detected nuclear magnetic resonance offer exquisite sensitivity to absolute shifts in spin transition frequencies, with potential applications in fundamental physics experiments and inertial sensing. We investigate 13C nuclear spins in diamond as a candidate system for solid-state implementations, which hold the promise for high-fidelity readout of large numbers of coherent nuclear spins in millitesla or lower magnetic fields. We demonstrate a technique that allows for both optical polarization and readout of large ensembles of ~10^{16} polarized nuclear spins. Our method takes advantage of state-selective Landau-Zener transitions under microwave frequency sweeping, which bidirectionally transfer spin polarization between Nitrogen-Vacancy (NV) electron spins and remote 13C nuclear spins. Using natural isotopic abundance diamonds with nitrogen densities of ~0.5-10 ppm, we perform optically-detected 13C Ramsey spectroscopy and realize a nuclear-spin-dependent fluorescence contrast exceeding 0.5% peak-to-peak. We observe nuclear spin dephasing times T2*~2 ms that only modestly improve with homonuclear dipolar decoupling, indicating that they are limited by the longitudinal spin relaxation of nearby NV electron spins. We study the magnetic field dependence of the optical readout and find comparable contrast and dephasing times for magnetic fields in the range 8-20 mT. Our method can be interpreted as a type of repetitive readout, where each NV center optically reads out the spin state of ~100 nuclei before nuclear spins depolarize.

quant-ph↗

arXiv2026

Orbital glass conceals missing magnetic entropy in a relativistic Mott insulator

Coupling between different degrees of freedom (DOF) in an electronic material leads to exotic phases of matter characterized by complex and competing order parameters as well as emergent excitations. Building a microscopic understanding of these order parameters and their mutual relationship is hindered by the fact that different orders often mask each others' response to conventional experimental probes. Here, we reveal how to disentangle responses from distinct orders that arise from the coupling between the spin and orbital DOF. Our method uses a phase sensitive technique that measures ground state properties by independently resolving interactions of different symmetries. This allows us to directly detect an orbital glass state caused by competing interactions in the $5d^1$ relativistic Mott insulator Ba$_2$NaOsO$_6$. We observe short-range orbital order up to 380 K and a dramatic increase of orbital dispersion near the magnetic phase transition. This orbital dispersion generates a directional ordering, $\textit{i.e.}$, it forms an orbital nematic state which breaks the rotational symmetry of the crystal. We establish that the orbital nematic state induces the magnetic ordering. The presence of this short-range orbital order well above the magnetic phase transition solves the long-standing puzzle of missing entropy in this material.

cond-mat.str-el↗

arXiv2026

Dynamic Simulations of Strongly Coupled Spin Ensembles for Inferring Nature of Electronic Correlations from Nuclear Magnetic Resonance

We develop an efficient package for the simulation of nuclear magnetic resonance spin echo experiments to study the effects of strong electronic spin correlations on the dynamics of the nuclear spin ensemble. A mean-field model is used to study correlated electronic phases through their hyperfine interaction with nuclear spins. We explore the dynamics of the interacting nuclear ensemble and discuss the key behaviors of the system. In particular, we classify the types of temporal asymmetry that the interaction induces in the system as well as a pulse-dependent shift in the spectral domain. Using these results, we discuss how careful measurement of the pulse-dependent shift can be used to extract information about the anisotropy of the electronic interaction and how these results represent a novel tool for the examination of exotic NMR signatures in strongly correlated materials. Finally, we review specific aspects of the simulation package developed for our exploration and give explicit examples where package can be used to infer range and anisotropy of electronic correlations. In particular, we discuss its structure, accuracy, and the technical merits of the various approximations used to model the nuclear spin ensemble.

cond-mat.str-el↗

arXiv2025

Exploring Overlapping Mechanisms of Dynamic Nuclear Polarization in Type 1b HPHT Diamond

The inhomogeneous distribution of P1 centers in type 1b HPHT diamond samples allows multiple DNP mechanisms to occur within the same crystal, resulting in complex DNP spectra. At some crystal orientations, different DNP mechanisms can compete to drive hyperpolarization with different signs at the same applied microwave frequency. We perform microwave-irradiated DNP using both monochromatic and frequency-modulated microwave excitation to explore the competition between these DNP mechanisms in diamond at room temperature. We demonstrate that frequency-modulated DNP is a tool for suppressing certain DNP mechanisms while enhancing others in a single-crystal diamond sample. Frequency modulation also enables higher enhancement of the NMR signal beyond traditional monochromatic DNP under some conditions. In a powder sample, competing enhancement mechanisms can also arise from different crystallite orientations in the powder. We observe that at certain microwave frequencies the DNP signal changes sign during the polarization build-up, even with monochromatic microwave irradiation. We do not observe this phenomenon in any single-crystal spectrum. We discuss both methods of investigating competing mechanisms of DNP as a means of selectively enhancing different DNP mechanisms driving $^{13}$C NMR signal enhancement.

physics.chem-ph↗

arXiv2025

Generation of Ultrahigh Anomalous Hall Conductivities via Optimally Prepared Topological Floquet States

Ultrafast quantum matter experiments have validated predictions from Floquet theory - notably, the dynamical modification of the electronic band structure and the light-induced anomalous Hall effect, via monotonic modulation of the driving amplitude. Here, we demonstrate how new physics is uncovered by leveraging quantum optimal control techniques to design Floquet amplitude modulation profiles. We discover a fundamentally different regime of topological transport, whereby the optimal oscillatory preparation protocol functions as a non-adiabatic topological pump: as a result, ultrahigh time-averaged anomalous Hall conductivities emerge, that reach up to around seventy times the values one would expect from the Chern number of the targeted Floquet state. The optimal protocols achieve >99% fidelity at the topological energy gap closing point - a twenty-fold improvement over standard monotonic approaches in as little as ten Floquet cycles - while unexpectedly generating the predicted ultrahigh conductivities. Our findings demonstrate that optimally prepared non-equilibrium quantum states can access transport regimes not achievable in the corresponding equilibrium system or even by applying conventional Floquet approaches, opening new avenues for ultrafast quantum technologies and topological device applications.

cond-mat.mes-hall↗

arXiv2024

Decoupling Dipolar Interactions in Dense Spin Ensembles

Dense spin ensembles in solids present a natural platform for studying quantum many-body dynamics. Multiple-pulse coherent control can be used to manipulate the magnetic dipolar interaction between the spins to engineer their dynamics. Here, we investigate the performance of a series of well-known pulse sequences that aim to suppress inter-spin dipolar couplings. We use a combination of numerical simulations and solid-state nuclear magnetic resonance (NMR) experiments on adamantane to evaluate and compare sequence performance. We study the role of sequence parameters like inter-pulse delays and resonance offsets. Disagreements between experiments and theory are typically explained by the presence of control errors and experimental non-idealities. The simulations allow us to explore the influence of factors such as finite pulse widths, rotation errors, and phase transient errors. We also investigate the role of local disorder and establish that it is, perhaps unsurprisingly, a distinguishing factor in the decoupling efficiency of spectroscopic sequences (that preserve Hamiltonian terms proportional to $S_z$) and time-suspension sequences (which refocus all terms in the internal Hamiltonian). We discuss our findings in the context of previously known analytical results from Average Hamiltonian Theory. Finally, we explore the ability of time-suspension sequences to protect multi-spin correlations in the system.

quant-ph↗

arXiv2024

Characterizing the magnetic noise power spectrum of dark spins in diamond

Coherence times of spin qubits in solid-state platforms are often limited by the presence of a spin bath. While some properties of these typically dark bath spins can be indirectly characterized via the central qubit, it is important to characterize their properties by direct measurement. Here we use pulsed electron paramagnetic resonance (pEPR) based Carr-Purcell-Meiboom-Gill (CPMG) dynamical decoupling to measure the magnetic noise power spectra for ensembles of P1 (substitutional nitrogen) centers in diamond that typically form the bath for NV (nitrogen-vacancy) centers. The experiments on the P1 centers were performed on a low [N] CVD (chemical vapor deposition) sample and a high [N] HPHT (high-temperature, high-pressure) sample at 89 mT. We characterize the NV centers of the latter sample using the same 2.5 GHz pEPR spectrometer. All power spectra show two distinct features, a broad component that is observed to scale as approximately $1/ω^{0.7-1.0}$, and a prominent peak at the $^{13}$C Larmor frequency. The behavior of the broad component is consistent with an inhomogeneous distribution of Lorentzian spectra due to clustering of P1 centers, which has recently been shown to be prevalent in HPHT diamond. It is unknown if such clustering occurs in CVD diamond. We develop techniques utilizing harmonics of the CPMG filter function to improve characterization of high-frequency signals, which we demonstrate on the $^{13}$C nuclear Larmor frequency. At 190 mT this is 2.04 MHz, 5.7 times higher than the CPMG modulation frequency ($<357$ kHz, hardware-limited). We assess the robustness of our methods in the presence of finite pulse widths and flip angle errors. Understanding the interactions of dark spins will inform methods of diamond fabrication for quantum technology. These techniques are applicable to ac magnetometry for nanoscale nuclear magnetic resonance and chemical sensing.

quant-ph↗

arXiv2023

P1 center electron spin clusters are prevalent in type Ib diamond

Understanding the spatial distribution of P1 centers is crucial for diamond-based sensors and quantum devices. P1 centers serve as a polarization source for DNP quantum sensing and play a significant role in the relaxation of NV centers. Additionally, the distribution of NV centers correlates with the distribution of P1 centers, as NV centers are formed through the conversion of P1 centers. We utilized dynamic nuclear polarization (DNP) and pulsed electron paramagnetic resonance (EPR) techniques that revealed strong clustering of a significant population of P1 centers that exhibit exchange coupling and produce asymmetric lineshapes. The $^{13}$C DNP frequency profile at high magnetic field revealed a pattern that requires an asymmetric EPR lineshape of the P1 clusters with electron-electron (e-e) coupling strengths exceeding the $^{13}$C nuclear Larmor frequency. EPR and DNP characterization at high magnetic fields was necessary to resolve energy contributions from different e-e couplings. We employed a two-frequency pump-probe pulsed Electron Double Resonance (ELDOR) technique to show crosstalk between the isolated and clustered P1 centers. This finding implies that the clustered P1 centers affect all P1 populations. Direct observation of clustered P1 centers and their asymmetric lineshape is a novel and crucial insight into understanding magnetic noise sources for quantum information applications of diamonds and for designing diamond-based polarizing agents with optimized DNP efficiency for $^{13}$C and other nuclear spins of analytes. We propose that room temperature $^{13}$C DNP at high field, achievable through straightforward modifications to existing solution-state NMR systems, is a potent tool for evaluating and controlling diamond defects.

physics.chem-ph↗

arXiv2023

Optical Conductivity Signatures of Floquet Electronic Phases

Optical conductivity measurements may provide access to distinct signatures of Floquet electronic phases, which are described theoretically by their quasienergy band structures. We characterize experimental observables of the Floquet graphene antidot lattice (FGAL), which we introduced previously [Phys. Rev. B 104, 174304 (2021)]. On the basis of Floquet linear response theory, the real and imaginary parts of the longitudinal and Hall optical conductivity are computed as a function of probe frequency. We find that the number and positions of peaks in the response function are distinctive of the different Floquet electronic phases, and identify multiple properties with no equilibrium analog. First, for several intervals of probe frequencies, the real part of the conductivity becomes negative. We argue this is indicative of a subversion of the usual Joule heating mechanism: The Floquet drive causes the material to amplify the power of the probe, resulting in gain. Additionally, while the Hall response vanishes at equilibrium, the real and imaginary parts of the Floquet Hall conductivity are non-zero and can be as large as the longitudinal components. Lastly, driving-induced localization tends to reduce the overall magnitude of and to flatten out the optical conductivity signal. From an implementation standpoint, a major advantage of the FGAL is that the above-bandwidth driving limit is reached with photon energies that are at least twenty times lower than that required for the intrinsic material, allowing for significant band renormalization at orders-of-magnitude smaller intensities. Our work provides the necessary tools for experimentalists to map reflectance data to particular Floquet phases for this novel material.

cond-mat.mes-hall↗

arXiv2023

Machine learning assisted determination of electronic correlations from magnetic resonance

In the presence of strong electronic spin correlations, the hyperfine interaction imparts long-range coupling between nuclear spins. Efficient protocols for the extraction of such complex information about electron correlations via magnetic response are not well known. Here, we study how machine learning can extract material parameters and help interpret magnetic response experiments. A low-dimensional representation that classifies the total interaction strength is discovered by unsupervised learning. Supervised learning generates models that predict the spatial extent of electronic correlations and the total interaction strength. Our work demonstrates the utility of artificial intelligence in the development of new probes of quantum systems, with applications to experimental studies of strongly correlated materials.

cond-mat.dis-nn↗

arXiv2023

Multi-modal spectroscopy of order parameter distributions

We present a multi-modal spectroscopic paradigm that enables independent measurement of charge and spin degrees of freedom (DOF) in strongly correlated materials. This spin-based technique probes symmetry-specific Hamiltonian parameters by analyzing how the time delay between applied pulses ($τ$) affects the response. We demonstrate ways in which charge DOF that couple through the quadrupolar interaction (inversion symmetric) can be independently measured even in the presence of large magnetic noise (inversion asymmetric). The method quantifies both the strength of the interactions and its distribution (noise). We provide protocols to directly and independently measure the distribution of interaction strengths, even when the average value of the interaction is zero. By independently measuring distributions of different forms of disorder, this methodology can elucidate which microscopic symmetry drives a phase transition. We discuss potential applications to study complex phase transitions in strongly interacting quantum materials.

cond-mat.mes-hall↗

arXiv2022

Spin Squeezing as a Probe of Emergent Quantum Orders

Nuclear magnetic resonance (NMR) experiments can reveal local properties in materials, but are often limited by the low signal-to-noise ratio. Spin squeezed states have an improved resolution below the Heisenberg limit in one of the spin components, and have been extensively used to improve the sensitivity of atomic clocks, for example. Interacting and entangled spin ensembles with non-linear coupling are a natural candidate for implementing squeezing. Here, we propose measurement of the spin-squeezing parameter that itself can act as a local probe of emergent orders in quantum materials. In particular, we demonstrate how to investigate an anisotropic electric field gradient via its coupling to the nuclear quadrupole moment. While squeezed spin states are pure, the squeezing parameter can be estimated for both pure and mixed states. We evaluate the range of fields and temperatures for which a thermal-equilibrium state is sufficient to improve the resolution in an NMR experiment and probe relevant parameters of the quadrupole Hamiltonian, including its anisotropy.

quant-ph↗

arXiv2022

Room Temperature DNP of Diamond Powder Using Frequency Modulation

Dynamic nuclear polarization (DNP) is a method of enhancing NMR signals via the transfer of polarization from electron spins to nuclear spins using on-resonance microwave (MW) irradiation. In most cases, monochromatic continuous-wave (MCW) MW irradiation is used. Recently, several groups have shown that the use of frequency modulation of the MW irradiation can result in an additional increase in DNP enhancement above that obtained with MCW. The effect of frequency modulation on the solid effect (SE) and the cross effect (CE) has previously been studied using the stable organic radical 4-hydroxy TEMPO (TEMPOL) at temperatures under 20 K. Here, in addition to the SE and CE, we discuss the effect of frequency modulation on the Overhauser effect (OE) and the truncated CE (tCE) in the room-temperature $^{13}$C-DNP of diamond powders. We recently showed that diamond powders can exhibit multiple DNP mechanisms simultaneously due to the heterogeneity of P1 (substitutional nitrogen) environments within diamond crystallites. We explore the enhancement obtained via the two most important parameters for frequency modulation 1) Modulation frequency, $f_{m}$ (how fast the modulation frequency is varied) and 2) Modulation amplitude, $Δω$ (the magnitude of the change in microwave frequency) influence the enhancement obtained via each mechanism. Frequency modulation during DNP not only allows us to improve DNP enhancement, but also gives us a way to control which DNP mechanism is most active. By choosing the appropriate modulation parameters, we can selectively enhance some mechanisms while simultaneously suppressing others.

physics.chem-ph↗

arXiv2022

Large Room Temperature Bulk DNP of $^{13}$C via P1 Centers in Diamond

We use microwave-induced dynamic nuclear polarization (DNP) of the substitutional nitrogen defects (P1 centers) in diamond to hyperpolarize bulk $^{13}$C nuclei in both single crystal and powder samples at room temperature at 3.34 T. The large ($>100$-fold) enhancements demonstrated correspond to a greater than 10,000 fold improvement in terms of signal averaging of the 1\% abundant $^{13}$C spins. The DNP was performed using low-power solid state sources under static (non-spinning) conditions. The DNP spectrum (DNP enhancement as a function of microwave frequency) of diamond powder shows features that broadly correlate with the EPR spectrum. A well-defined negative Overhauser peak and two solid effect peaks are observed for the central ($m_I=0$) manifold of the $^{14}$N spins. Previous low temperature measurements in diamond had measured a positive Overhauser enhancement in this manifold. Frequency-chirped millimeter-wave excitation of the electron spins is seen to significantly improve the enhancements for the two outer nuclear spin manifolds ($m_I = \pm 1$) and to blur some of the sharper features associated with the central manifolds. The outer lines are best fit using a combination of the cross effect and a truncated cross effect -- which is known to mimic features of an Overhauser effect. Similar features are also observed in experiments on single crystal samples. The observation of all of these mechanisms in a single material system under the same experimental conditions is likely due to the significant heterogeneity of the high pressure, high temperature (HPHT) type Ib diamond samples used. Large room temperature DNP enhancements at fields above a few Tesla enable spectroscopic studies with better chemical shift resolution under ambient conditions.

cond-mat.mtrl-sci↗

arXiv2021

Floquet Graphene Antidot Lattices

We establish the theoretical foundation of the Floquet graphene antidot lattice, whereby massless Dirac fermions are driven periodically by a circularly polarized electromagnetic field, while having their motion excluded from an array of nanoholes. The properties of interest are encoded in the quasienergy spectra, which are computed non-perturbatively within the Floquet formalism. We find that a rich Floquet phase diagram emerges as the amplitude of the drive field is varied. Notably, the Dirac dispersion can be restored in real time relative to the gapped equilibrium state, which may enable the creation of an optoelectronic switch or a dynamically tunable electronic waveguide. As the amplitude is increased, the ability to shift the quasienergy gap between high-symmetry points can change which crystal momenta dominate in the scattering processes relevant to electronic transport and optical emission. Furthermore, the bands can be flattened near the $Γ$ point, which is indicative of selective dynamical localization. Lastly, quadratic and linear dispersions emerge in orthogonal directions at the $M$ point, signaling a Floquet semi-Dirac material. Importantly, all our predictions are valid for experimentally accessible near-IR radiation, which corresponds to the above bandwidth limit for the graphene antidot lattice. Cycling between engineered Floquet electronic phases may play a key role in the development of next-generation on-chip devices for optoelectronic applications.

cond-mat.mes-hall↗

arXiv2021

Signatures of electronic correlations and spin-susceptibility anisotropy in nuclear magnetic resonance

We present a methodology for probing the details of electronic susceptibility through minimally-invasive nuclear magnetic resonance techniques. Specifically, we classify electron-mediated long-range interactions in an ensemble of nuclear spins by revealing their effect on simple spin echo experiments. We find that pulse strength and applied field orientation dependence of these spin echo measurements resolves the spatial extent and anisotropy of electronic spin susceptibility. This work provides an alternate explanation to NMR results in superconducting and magnetically-ordered systems. The methodology has direct applications for sensing and characterizing emergent electronic phases.

cond-mat.str-el↗

arXiv2021

Spectral diffusion of phosphorus donors in silicon at high magnetic field

We characterize the phase memory time of phosphorus donor electron spins in lightly-doped natural silicon at high magnetic field (8.58 T) in the dark and under low-power optical excitation. The spin echo decays are dominated by spectral diffusion due to the presence of the 4.7% abundant spin-1/2 silicon-29 nuclei. At 4.2 K, the spectral diffusion time (T$_{SD}$) measured in the dark is $124 \pm 7$ $μ$s, a factor of 2 smaller than that measured at low magnetic fields (0.35 T). Using a tunable laser we also measured the echo decay as the wavelength of the optical excitation is swept across the band edge from 1050 nm to 1090 nm. Above-bandgap optical excitation is seen to increase the spectral diffusion time of the donor electron spin to $201 \pm 11$ $μ$s. The physical mechanism underlying both the decrease of T$_{SD}$ at high field and the subsequent increase under optical excitation remains unclear.

quant-ph↗

arXiv2021

Deep reinforcement learning for quantum Hamiltonian engineering

Engineering desired Hamiltonian in quantum many-body systems is essential for applications such as quantum simulation, computation and sensing. Conventional quantum Hamiltonian engineering sequences are designed using human intuition based on perturbation theory, which may not describe the optimal solution and is unable to accommodate complex experimental imperfections. Here we numerically search for Hamiltonian engineering sequences using deep reinforcement learning (DRL) techniques and experimentally demonstrate that they outperform celebrated sequences on a solid-state nuclear magnetic resonance quantum simulator. As an example, we aim at decoupling strongly-interacting spin-1/2 systems. We train DRL agents in the presence of different experimental imperfections and verify robustness of the output sequences both in simulations and experiments. Surprisingly, many of the learned sequences exhibit a common pattern that had not been discovered before, to our knowledge, but has an meaningful analytical description. We can thus restrict the searching space based on this control pattern, allowing to search for longer sequences, ultimately leading to sequences that are robust against dominant imperfections in our experiments. Our results not only demonstrate a general method for quantum Hamiltonian engineering, but also highlight the importance of combining black-box artificial intelligence with understanding of physical system in order to realize experimentally feasible applications.

quant-ph↗