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Prineha Narang

Publications and source records attributed to Prineha Narang.

At least 109 records · Page 6Linked to original sources

Challenges in Plasmonic Catalysis

The use of nanoplasmonics to control light and heat close to the thermodynamic limit enables exciting opportunities in the field of plasmonic catalysis. The decay of plasmonic excitations creates highly nonequilibrium distributions of hot carriers that can initiate or catalyze reactions through both thermal and nonthermal pathways. In this Perspective, we present the current understanding in the field of plasmonic catalysis, capturing vibrant debates in the literature, and discuss future avenues of exploration to overcome critical bottlenecks. Our Perspective spans first-principles theory and computation of correlated and far-from-equilibrium light-matter interactions, synthesis of new nanoplasmonic hybrids, and new steady-state and ultrafast spectroscopic probes of interactions in plasmonic catalysis, recognizing the key contributions of each discipline in realizing the promise of plasmonic catalysis. We conclude with our vision for fundamental and technological advances in the field of plasmon-driven chemical reactions in the coming years.

physics.optics↗

Building a Quantum Engineering Undergraduate Program

The rapidly growing quantum information science and engineering (QISE) industry will require both quantum-aware and quantum-proficient engineers at the bachelor's level. We provide a roadmap for building a quantum engineering education program to satisfy this need. For quantum-aware engineers, we describe how to design a first quantum engineering course accessible to all STEM students. For the education and training of quantum-proficient engineers, we detail both a quantum engineering minor accessible to all STEM majors, and a quantum track directly integrated into individual engineering majors. We propose that such programs typically require only three or four newly developed courses that complement existing engineering and science classes available on most larger campuses. We describe a conceptual quantum information science course for implementation at any post-secondary institution, including community colleges and military schools. QISE presents extraordinary opportunities to work towards rectifying issues of inclusivity and equity that continue to be pervasive within engineering. We present a plan to do so and describe how quantum engineering education presents an excellent set of education research opportunities. Finally, we outline a hands-on training plan on quantum hardware, a key component of any quantum engineering program, with a variety of technologies including optics, atoms and ions, cryogenic and solid-state technologies, nanofabrication, and control and readout electronics. Our recommendations provide a flexible framework that can be tailored for academic institutions ranging from teaching and undergraduate-focused two- and four-year colleges to research-intensive universities.

physics.ed-ph↗

Atomistic spin textures on-demand in the van der Waals layered magnet CrSBr

Controlling magnetism in low dimensional materials is essential for designing devices that have feature sizes comparable to several critical length scales that exploit functional spin textures, allowing the realization of low-power spintronic and magneto-electric hardware. [1] Unlike conventional covalently-bonded bulk materials, van der Waals (vdW)-bonded layered magnets [2-4] offer exceptional degrees of freedom for engineering spin textures. [5] However, their structural instability has hindered microscopic studies and manipulations. Here, we demonstrate nanoscale structural control in the layered magnet CrSBr creating novel spin textures down to the atomic scale. We show that it is possible to drive a local structural phase transformation using an electron beam that locally exchanges the bondings in different directions, effectively creating regions that have vertical vdW layers embedded within the horizontally vdW bonded exfoliated flakes. We calculate that the newly formed 2D structure is ferromagnetically ordered in-plane with an energy gap in the visible spectrum, and weak antiferromagnetism between the planes. Our study lays the groundwork for designing and studying novel spin textures and related quantum magnetic phases down to single-atom sensitivity, potentially to create on-demand spin Hamiltonians probing fundamental concepts in physics, [6-10] and for realizing high-performance spintronic, magneto-electric and topological devices with nanometer feature sizes. [11,12]

cond-mat.mes-hall↗

Spectroscopic signatures of time-reversal symmetry breaking superconductivity

The collective mode spectrum of a symmetry-breaking state, such as a superconductor, provides crucial insight into the nature of the order parameter. In this context, we present a microscopic weak-coupling theory for the collective modes of a generic multi-component time-reversal symmetry breaking superconductor, and show that fluctuations in the relative amplitude and phase of the two order parameter components are well-defined underdamped collective modes, even in the presence of nodal quasiparticles. We then demonstrate that these "generalized clapping modes" can be detected using a number of experimental techniques including ac electronic compressibility measurements, electron energy loss spectroscopy, microwave spectroscopy, and ultrafast THz spectroscopy. Finally, we discuss the implications of our work as a new form of "collective mode spectroscopy" that drastically expands the number of experimental probes capable of detecting time-reversal symmetry breaking in unconventional superconductors such as Sr$_{\text{2}}$RuO$_{\text{4}}$, UTe$_{\text{2}}$, and moiré heterostructures.

cond-mat.supr-con↗

Quantum Simulation of Open Quantum Systems Using a Unitary Decomposition of Operators

Electron transport in realistic physical and chemical systems often involves the non-trivial exchange of energy with a large environment, requiring the definition and treatment of open quantum systems. Because the time evolution of an open quantum system employs a non-unitary operator, the simulation of open quantum systems presents a challenge for universal quantum computers constructed from only unitary operators or gates. Here we present a general algorithm for implementing the action of any non-unitary operator on an arbitrary state on a quantum device. We show that any quantum operator can be exactly decomposed as a linear combination of at most four unitary operators. We demonstrate this method on a two-level system in both zero and finite temperature amplitude damping channels. The results are in agreement with classical calculations, showing promise in simulating non-unitary operations on intermediate-term and future quantum devices.

quant-ph↗

Cavity magnon-polaritons in cuprate parent compounds

Cavity control of quantum matter may offer new ways to study and manipulate many-body systems. A particularly appealing idea is to use cavities to enhance superconductivity, especially in unconventional or high-$T_c$ systems. Motivated by this, we propose a scheme for coupling Terahertz resonators to the antiferromagnetic fluctuations in a cuprate parent compound, which are believed to provide the glue for Cooper pairs in the superconducting phase. First, we derive the interaction between magnon excitations of the Neél-order and polar phonons associated with the planar oxygens. This mode also couples to the cavity electric field, and in the presence of spin-orbit interactions mediates a linear coupling between the cavity and magnons, forming hybridized magnon-polaritons. This hybridization vanishes linearly with photon momentum, implying the need for near-field optical methods, which we analyze within a simple model. We then derive a higher-order coupling between the cavity and magnons which is only present in bilayer systems, but does not rely on spin-orbit coupling. This interaction is found to be large, but only couples to the bimagnon operator. As a result we find a strong, but heavily damped, bimagnon-cavity interaction which produces highly asymmetric cavity line-shapes in the strong-coupling regime. To conclude, we outline several interesting extensions of our theory, including applications to carrier-doped cuprates and other strongly-correlated systems with Terahertz-scale magnetic excitations.

cond-mat.str-el↗

Finite-size effects of electron transport in PdCoO$_2$

A wide range of unconventional transport phenomena have recently been observed in single-crystal delafossite metals. Here, we present a theoretical framework to elucidate electron transport using a combination of first-principles calculations and numerical modeling of the anisotropic Boltzmann transport equation. Using PdCoO$_2$ as a model system, we study different microscopic electron and phonon scattering mechanisms and establish the mean free path hierarchy of quasiparticles at different temperatures. We treat the anisotropic Fermi surface explicitly to numerically obtain experimentally-accessible transport observables, which bridge between the "diffusive", "ballistic", and "hydrodynamic" transport regime limits. We illustrate that distinction between the "quasi-ballistic", and "quasi-hydrodynamic" regimes is challenging and often needs to be quantitative in nature. From first-principles calculations, we populate the resulting transport regime plots, and demonstrate how the Fermi surface orientation adds complexity to the observed transport signatures in micro-scale devices. Our work provides key insights into microscopic interaction mechanisms on open hexagonal Fermi surfaces and establishes their connection to the macroscopic electron transport in finite-size channels.

cond-mat.mtrl-sci↗

Capturing 3D atomic defects and phonon localization at the 2D heterostructure interface

The 3D local atomic structures and crystal defects at the interfaces of heterostructures control their electronic, magnetic, optical, catalytic and topological quantum properties, but have thus far eluded any direct experimental determination. Here we determine the 3D local atomic positions at the interface of a MoS2-WSe2 heterojunction with picometer precision and correlate 3D atomic defects with localized vibrational properties at the epitaxial interface. We observe point defects, bond distortion, atomic-scale ripples and measure the full 3D strain tensor at the heterointerface. By using the experimental 3D atomic coordinates as direct input to first principles calculations, we reveal new phonon modes localized at the interface, which are corroborated by spatially resolved electron energy-loss spectroscopy. We expect that this work will open the door to correlate structure-property relationships of a wide range of heterostructure interfaces at the single-atom level.

cond-mat.mtrl-sci↗

Room temperature single-photon superfluorescence from a single epitaxial cuboid nano-heterostructure

Single-photon superradiance can emerge when a collection of identical emitters are spatially separated by distances much less than the wavelength of the light they emit, and is characterized by the formation of a superradiant state that spontaneously emits light with a rate that scales linearly with the number of emitters. This collective phenomena has only been demonstrated in a few nanomaterial systems, all requiring temperatures below 10K. Here, we rationally design a single colloidal nanomaterial that hosts multiple (nearly) identical emitters that are impervious to the fluctuations which typically inhibit room temperature superradiance in other systems such as molecular aggregates. Specifically, by combining molecular dynamics, atomistic electronic structure calculations, and model Hamiltonian methods, we show that the faces of a heterostructure nanocuboid mimic individual quasi-2D nanoplatelets and can serve as the robust emitters required to realize superradiant phenomena at room temperature. Leveraging layer-by-layer colloidal growth techniques to synthesize a nanocuboid, we demonstrate single-photon superfluorescence via single-particle time-resolved photoluminescence measurements at room temperature. This robust observation of both superradiant and subradiant states in single nanocuboids opens the door to ultrafast single-photon emitters and provides an avenue to entangled multi-photon states via superradiant cascades.

physics.optics↗

Highly confined phonon polaritons in monolayers of oxide perovskites

Two-dimensional (2D) materials are able to strongly confine light hybridized with collective excitations of atoms, enabling electric-field enhancements and novel spectroscopic applications. Recently, freestanding monolayers of oxide perovskites have been synthesized, which possess highly infrared-active phonon modes and a complex interplay of competing interactions. In this study, we evaluate central figures of merit for phonon polaritons in the tetragonal phases of the 2D perovskites SrTiO$_3$, KTaO$_3$, and LiNbO$_3$, using density functional theory calculations. Specifically, we compute the 2D phonon-polariton dispersions, the propagation-quality, confinement, and deceleration factors, and we show that they are comparable to those found in the prototypical 2D dielectric hexagonal boron nitride. Our results suggest that monolayers of oxide perovskites are promising candidates for polaritonic platforms in the terahertz spectral range that enable possibilites to control complex phases of matter through strongly enhanced electromagnetic fields.

cond-mat.mtrl-sci↗

Demonstration of quantum advantage by a joint detection receiver for optical communications using quantum belief propagation on a trapped-ion device

Demonstrations of quantum advantage have largely focused on computational speedups and on quantum simulation of many-body physics, limited by fidelity and capability of current devices. Discriminating laser-pulse-modulated classical-communication codewords at the minimum allowable probability of error using universal-quantum processing presents a promising parallel direction, one that is of both fundamental importance in quantum state discrimination, as well as of technological relevance in deep-space laser communications. Here we present an experimental realization of a quantum joint detection receiver for binary phase shift keying modulated codewords of a 3-bit linear tree code using a recently-proposed quantum algorithm: belief propagation with quantum messages. The receiver, translated to a quantum circuit, was experimentally implemented on a trapped-ion device -- the recently released Honeywell LT-1.0 system using ${}^{171}Yb+ $ ions, which possesses all-to-all connectivity and mid-circuit measurement capabilities that are essential to this demonstration. We conclusively realize a previously postulated but hitherto not-demonstrated joint quantum detection scheme, and provide an experimental framework that surpasses the quantum limit on the minimum average decoding error probability associated with pulse-by-pulse detection in the low mean photon number limit. The full joint-detection scheme bridges across photonic and trapped-ion based quantum information science, mapping the photonic coherent states of the modulation alphabet onto inner product-preserving states of single-ion qubits. Looking ahead, our work opens new avenues in hybrid realizations of quantum-enhanced receivers with applications in astronomy and emerging space-based platforms.

quant-ph↗

Spin-Dependent Transport Through a Colloidal Quantum Dot: The Role of Exchange Interactions

The study of charge and spin transport through semiconductor quantum dots is experiencing a renaissance due to recent advances in nano-fabrication and the realization of quantum dots as candidates for quantum computing. In this work, we combine atomistic electronic structure calculations with quantum master equation methods to study the transport of electrons and holes through strongly confined quantum dots coupled to two leads with a voltage bias. We find that a competition between the energy spacing between the two lowest quasiparticle energy levels and the strength of the exchange interaction determines the spin states of the lowest two quasiparticle energy levels. Specifically, the low density of electron states results in a spin singlet being the lowest energy two-electron state whereas, in contrast, the high density of states and significant exchange interaction results in a spin triplet being the lowest energy two-hole state. The exchange interaction is also responsible for spin blockades in transport properties, which could persist up to temperatures as high as 77K for strongly confined colloidal quantum dots from our calculations. Lastly, we relate these findings to the preparation and manipulation of singlet and triplet spin qubit states in quantum dots using voltage biases.

cond-mat.mes-hall↗

Room-Temperature Photonic Logical Qubits via Second-Order Nonlinearities

Recent progress in nonlinear optical materials and microresonators has brought quantum computing with bulk optical nonlinearities into the realm of possibility. This platform is of great interest, not only because photonics is an obvious choice for quantum networks, but also because it may be the only feasible route to quantum information processing at room temperature. We introduce a paradigm for room-temperature photonic quantum logic that significantly simplifies the realization of various quantum circuits, and in particular, of error correction. It uses only the strongest available bulk nonlinearity, namely the $χ^{(2)}$ nonlinear susceptibility. The key element is a three-mode resonator that implements programmable bosonic quantum logic gates. We show that just two of these elements suffice for a complete, compact error-correction circuit on a bosonic code, without the need for measurement or feed-forward control. An extrapolation of current progress in nonlinear optical materials and photonic circuits indicates that such circuitry should be achievable within the next decade.

quant-ph↗

Branching Quantum Convolutional Neural Networks

Neural network-based algorithms have garnered considerable attention in condensed matter physics for their ability to learn complex patterns from very high dimensional data sets towards classifying complex long-range patterns of entanglement and correlations in many-body quantum systems. Small-scale quantum computers are already showing potential gains in learning tasks on large quantum and very large classical data sets. A particularly interesting class of algorithms, the quantum convolutional neural networks (QCNN) could learn features of a quantum data set by performing a binary classification task on a nontrivial phase of quantum matter. Inspired by this promise, we present a generalization of QCNN, the branching quantum convolutional neural network, or bQCNN, with substantially higher expressibility. A key feature of bQCNN is that it leverages mid-circuit (intermediate) measurement results, realizable on current trapped-ion systems, obtained in pooling layers to determine which sets of parameters will be used in the subsequent convolutional layers of the circuit. This results in a branching structure, which allows for a greater number of trainable variational parameters in a given circuit depth. This is of particular use on current-day NISQ devices, where circuit depth is limited by gate noise. We present an overview of the ansatz structure and scaling, and provide evidence of its enhanced expressibility compared to QCNN. Using artificially-constructed large data sets of training states as a proof-of-concept we demonstrate the existence of training tasks in which bQCNN far outperforms an ordinary QCNN. Finally, we present future directions where the classical branching structure and increased density of trainable parameters in bQCNN would be particularly valuable.

quant-ph↗

Hybridized defects in solid-state materials as artificial molecules

Two-dimensional materials can be crafted with structural precision approaching the atomic scale, enabling quantum defects-by-design. These defects are frequently described as artificial atoms and are emerging optically-addressable spin qubits. However, interactions and coupling of such artificial atoms with each other, in the presence of the lattice, is remarkably underexplored. Here we present the formation of artificial molecules in solids, introducing a new degree of freedom in control of quantum optoelectronic materials. Specifically, in monolayer hexagonal boron nitride as our model system, we observe configuration- and distance-dependent dissociation curves and hybridization of defect orbitals within the bandgap into bonding and antibonding orbitals, with splitting energies ranging from $\sim$ 10 meV to nearly 1 eV. We calculate the energetics of $cis$ and $trans$ out-of-plane defect pairs CH$_\textrm{B}$-CH$_\textrm{B}$ against an in-plane defect pair C$_\textrm{B}$-C$_\textrm{B}$ and find that in-plane defect pair interacts more strongly than out-of-plane pairs. We demonstrate an application of this chemical degree of freedom by varying the distance between C$_\textrm{B}$ and V$_\textrm{N}$ of C$_\textrm{B}$V$_\textrm{N}$ and observe changes in the predicted peak absorption wavelength from the visible to the near-infrared spectral band. We envision leveraging this chemical degree of freedom of defect complexes to precisely control and tune defect properties towards engineering robust quantum memories and quantum emitters for quantum information science.

quant-ph↗

Anisotropic phonon-mediated electronic transport in chiral Weyl semimetals

Discovery and observations of exotic, quantized optical and electrical responses have sparked renewed interest in nonmagnetic chiral crystals. Within this class of materials, six group V transition metal ditetrelides, that is, XY$_2$ (X = V, Nb, Ta and Y = Si, Ge), host composite Weyl nodes on high-symmetry lines, with Kramers-Weyl fermions at time-reversal invariant momenta. In addition, at least two of these materials, NbGe$_2$ and NbSi$_2$, exhibit superconducting transitions at low temperatures. The interplay of strong electron-phonon interaction and complex Fermi surface topology present an opportunity to study both superconductivity and hydrodynamic electron transport in these systems. Towards this broader question, we present an ab initio theoretical study of the electronic transport and electron-phonon scattering in this family of materials, with a particular focus on NbGe$_2$ vs. NbSi$_2$, and the other group V ditetrelides. We shed light on the microscopic origin of NbGe$_2$'s large and anisotropic room temperature resistivity and contextualize its strong electron-phonon scattering with a presentation of other relevant scattering lifetimes, both momentum-relaxing and momentum-conserving. Our work explores the intriguing possibility of observing hydrodynamic electron transport in these chiral Weyl semimetals.

cond-mat.supr-con↗

Sondheimer oscillations as a probe of non-ohmic flow in type-II Weyl semimetal WP$_2$

As conductors in electronic applications shrink, microscopic conduction processes lead to strong deviations from Ohm's law. Depending on the length scales of momentum conserving ($l_{MC}$) and relaxing ($l_{MR}$) electron scattering, and the device size ($d$), current flows may shift from ohmic to ballistic to hydrodynamic regimes and more exotic mixtures thereof. So far, an in situ, in-operando methodology to obtain these parameters self-consistently within a micro/nanodevice, and thereby identify its conduction regime, is critically lacking. In this context, we exploit Sondheimer oscillations, semi-classical magnetoresistance oscillations due to helical electronic motion, as a method to obtain $l_{MR}$ in micro-devices even when $l_{MR}\gg d$. This gives information on the bulk $l_{MR}$ complementary to quantum oscillations, which are sensitive to all scattering processes. We extract $l_{MR}$ from the Sondheimer amplitude in the topological semi-metal WP$_2$, at elevated temperatures up to $T\sim 50$~K, in a range most relevant for hydrodynamic transport phenomena. Our data on micrometer-sized devices are in excellent agreement with experimental reports of the large bulk $l_{MR}$ and thus confirm that WP$_2$ can be microfabricated without degradation. Indeed, the measured scattering rates match well with those of theoretically predicted electron-phonon scattering, thus supporting the notion of strong momentum exchange between electrons and phonons in WP$_2$ at these temperatures. These results conclusively establish Sondheimer oscillations as a quantitative probe of $l_{MR}$ in micro-devices in studying non-ohmic electron flow.

cond-mat.mes-hall↗

Spin emitters beyond the point dipole approximation in nanomagnonic cavities

Control over transition rates between spin states of emitters is crucial in a wide variety of fields ranging from quantum information science to the nanochemistry of free radicals. We present an approach to drive a both electric and magnetic dipole-forbidden transition of a spin emitter by placing it in a nanomagnonic cavity, requiring a description of both the spin emitter beyond the point dipole approximation and the vacuum magnetic fields of the nanomagnonic cavity with a large spatial gradient over the volume of the spin emitter. We specifically study the SiV$^-$ defect in diamond, whose Zeeman-split ground states comprise a logical qubit for solid-state quantum information processing, coupled to a magnetic nanoparticle serving as a model nanomagnonic cavity capable of concentrating microwave magnetic fields into deeply subwavelength volumes. Through first principles modeling of the SiV$^-$ spin orbitals, we calculate the spin transition densities of magnetic dipole-allowed and -forbidden transitions and calculate their coupling rates to various multipolar modes of the nanomagnonic cavity. We envision using such a framework for quantum state transduction and state preparation of spin qubits at GHz frequency scales.

cond-mat.mes-hall↗