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Prineha Narang

Publications and source records attributed to Prineha Narang.

At least 91 records · Page 5Linked to original sources

Photoinduced Band Renormalization Effects in ZrSiS Topological Nodal-line Semimetal

Out-of-equilibrium effects provide an elegant pathway to probing and understanding the underlying physics of topological materials. Creating exotic states of matter using ultrafast optical pulses in particular has shown promise towards controlling electronic band structure properties. Of recent interest is band renormalization in Dirac and Weyl semimetals as it leads to direct physical observables through the enhancement of the effective mass, or, in the shift of resonant energies. Here we provide experimental and theoretical signatures of photo-induced renormalization of the electronic band structure in a topological nodal line semimetal ZrSiS. Specifically, we show how the change of the transient reflectivity spectra under femtosecond optical excitations is induced by out-of-equilibrium effects that renormalize the kinetic energy of electrons. We associate the observed spectral shift to an enhancement of the effective mass and to a red-shift of the resonant frequency as a function of pump field strength. Finally, we show that the transient relaxation dynamics of the reflectivity is primarily an electronic effect with negligible phononic contribution. Our study presents the modifications of electronic properties in ZrSiS using ultrashort pulses, and demonstrates the potential of this approach in creating photo-induced phases in topological quantum mater through an all-optical route.

cond-mat.mtrl-sci↗

Chemical reactions in imperfect cavities: enhancement, suppression, and resonance

The use of optical cavities to control chemical reactions has been of great interest recently, following demonstrations of enhancement, suppression, and negligible effects on chemical reaction rates depending on the specific reaction and cavity frequency. In this work, we study the reaction rate inside imperfect cavities, where we introduce a broadening parameter in the spectral density to mimic Fabry-Pérot cavities. We investigate cavity modifications to reaction rates using non-Markovian Langevin dynamics with frictional and random forces to account for the presence of imperfect optical cavities. We demonstrate that in the regime of weak solvent and cavity friction, the cavity can enhance chemical reaction rates. On the other hand, in the high friction regime, cavities can suppress chemical reactions. Furthermore, we find that the broadening of the cavity spectral density gives rise to blue shifts of the resonance conditions and, surprisingly, increases the sharpness of the resonance effect.

physics.chem-ph↗

Shining Light on the Microscopic Resonant Mechanism Responsible for Cavity-Mediated Chemical Reactivity

Strong light-matter interaction in cavity environments is emerging as a promising approach to control chemical reactions in a non-intrusive and efficient manner. The underlying mechanism that distinguishes between steering, accelerating, or decelerating a chemical reaction has, however, remained unclear, hampering progress in this frontier area of research. We leverage quantum-electrodynamical density-functional theory to unveil the microscopic mechanism behind the experimentally observed reduced reaction rate under cavity induced resonant vibrational strong light-matter coupling. We observe multiple resonances and obtain the thus far theoretically elusive but experimentally critical resonant feature for a single strongly-coupled molecule undergoing the reaction. While we do not explicitly account for collective coupling or intermolecular interactions, the qualitative agreement with experimental measurements suggests that our conclusions can be largely abstracted towards the experimental realization. Specifically, we find that the cavity mode acts as mediator between different vibrational modes. In effect, vibrational energy localized in single bonds that are critical for the reaction is redistributed differently which ultimately inhibits the reaction.

quant-ph↗

A general quantum algorithm for open quantum dynamics demonstrated with the Fenna-Matthews-Olson complex

Using quantum algorithms to simulate complex physical processes and correlations in quantum matter has been a major direction of quantum computing research, towards the promise of a quantum advantage over classical approaches. In this work we develop a generalized quantum algorithm to simulate any dynamical process represented by either the operator sum representation or the Lindblad master equation. We then demonstrate the quantum algorithm by simulating the dynamics of the Fenna-Matthews-Olson (FMO) complex on the IBM QASM quantum simulator. This work represents a first demonstration of a quantum algorithm for open quantum dynamics with a moderately sophisticated dynamical process involving a realistic biological structure. We discuss the complexity of the quantum algorithm relative to the classical method for the same purpose, presenting a decisive query complexity advantage of the quantum approach based on the unique property of quantum measurement.

quant-ph↗

Quantum State Preparation and Non-Unitary Evolution with Diagonal Operators

Realizing non-unitary transformations on unitary-gate based quantum devices is critically important for simulating a variety of physical problems including open quantum systems and subnormalized quantum states. We present a dilation based algorithm to simulate non-unitary operations using probabilistic quantum computing with only one ancilla qubit. We utilize the singular-value decomposition (SVD) to decompose any general quantum operator into a product of two unitary operators and a diagonal non-unitary operator, which we show can be implemented by a diagonal unitary operator in a 1-qubit dilated space. While dilation techniques increase the number of qubits in the calculation, and thus the gate complexity, our algorithm limits the operations required in the dilated space to a diagonal unitary operator, which has known circuit decompositions. We use this algorithm to prepare random sub-normalized two-level states on a quantum device with high fidelity. Furthermore, we present the accurate non-unitary dynamics of two-level open quantum systems in a dephasing channel and an amplitude damping channel computed on a quantum device. The algorithm presented will be most useful for implementing general non-unitary operations when the SVD can be readily computed, which is the case with most operators in the noisy intermediate-scale quantum computing era.

quant-ph↗

Probing carrier interactions using electron hydrodynamics

Electron hydrodynamics arises when momentum-relaxing scattering processes are slow compared to momentum-conserving ones. While the microscopic details necessary to satisfy this condition are material-specific, experimentally accessible current densities share remarkable similarities. We study the dependence of electron hydrodynamic flows on the rates of momentum-relaxing and momentum-conserving scattering processes in a microscopics-agnostic way. We develop a framework for generating random collision operators which respect crystal symmetries and conservation laws and which have a tunable ratio between the momentum-conserving and momentum-relaxing lifetimes. Using various random instances of these collision operators, we calculate macroscopic electron viscosity tensors and solve the Boltzmann transport equation (BTE) in a channel geometry over a grid of momentum-conserving and momentum-relaxing lifetimes, and for different crystal symmetry groups. We find that different random collision operators using the same lifetimes produce very similar current density profiles, meaning that the current density is primarily a probe of the overall rates of momentum conservation and relaxation. By contrast, the viscosity tensor varies substantially at fixed lifetimes, meaning that properties like channel resistance provide detailed probes of the underlying scattering processes. This suggests that, while details of the scattering process are imprinted in the electronic viscosity tensor, for many applications theoretical calculations of hydrodynamic electron flows can use experimentally-available lifetimes within a spatially-resolved BTE framework rather than requiring the costly computation of ab initio collision operators.

cond-mat.mtrl-sci↗

Tunable Nonlinearity and Efficient Harmonic Generation from a Strongly Coupled Light-Matter System

Strong light-matter coupling within electromagnetic environments provides a promising path to modify and control chemical and physical processes. The origin of the enhancement of nonlinear optical processes such as second-harmonic and third-harmonic generation (SHG and THG) due to strong light-matter coupling is attributed to distinct physical effects which questions the relevance of strong coupling in these processes. In this work, we leverage a first-principles approach to investigate the origins of the experimentally observed enhancement of resonant SHG and THG under strong light-matter coupling. We find that the enhancement of the nonlinear conversion efficiency has its origins in a modification of the associated nonlinear optical susceptibilities as polaritonic resonances emerge in the nonlinear spectrum. Further, we find that the nonlinear conversion efficiency can be tuned by increasing the light-matter coupling strength. Finally, we provide a general framework to compute the harmonic generation spectra from the displacement field as opposed to the standard approach which computes the harmonic spectrum from the matter-only induced polarization. Our results address a key debate in the field, and pave the way for predicting and understanding quantum nonlinear optical phenomena in strongly coupled light-matter systems.

physics.optics↗

Giant effective magnetic fields from optically driven chiral phonons in 4$f$ paramagnets

We present a mechanism by which optically driven chiral phonon modes in rare-earth trihalides generate giant effective magnetic fields acting on the paramagnetic $4f$ spins. With cerium trichloride (CeCl$_3$) as our example system, we calculate the coherent phonon dynamics in response to the excitation by an ultrashort terahertz pulse using a combination of phenomenological modeling and first-principles calculations. We find that effective magnetic fields of over 100 tesla can possibly be generated that polarize the spins for experimentally accessible pulse energies. The direction of induced magnetization can be reversed by changing the handedness of circular polarization of the laser pulse. The underlying process is a phonon analog of the inverse Faraday effect in optics that has been described recently, and which enables novel ways of achieving control over and switching of magnetic order at terahertz frequencies.

cond-mat.mtrl-sci↗

Nonlinear optical processes in centrosymmetric systems by strong-coupling-induced symmetry breaking

Nonlinear optical processes associated with even-order nonlinear susceptibilities are critical for both classical and quantum technologies. Inversion symmetry, however, prevents nonlinear optical responses mediated by even-order susceptibilities in several material systems pertinent for applications in nanophotonics. Here, we demonstrate induced nonlinear optical processes, namely second- and fourth-harmonic generation that are naturally forbidden in an inversion symmetric system, by strongly coupling to a photon mode of a high-Q optical cavity. As an illustrative system with an inversion symmetry, we consider a semiconductor quantum ring of GaAs that features a single effective electron. For the coupled system, we control the inversion symmetry breaking by changing the light-matter coupling strength which at the same time allows to tune the nonlinear conversion efficiency. We find that the harmonic generation yield can be significantly increased by increasing the light-matter coupling strength in an experimentally feasible way. In the few-photon limit where the incident pump field is a coherent state with just a few photons, we find that the harmonic conversion efficiency is increased for strong coupling as opposed to using intense pump fields. This new approach is applicable to a wide variety of centrosymmetric systems as the symmetry breaking rest on the properties of the photonic environment used to achieve strong light-matter interaction. Our work constitutes a step forward in the direction of realizing physically forbidden nonlinear optical processes in centrosymmetric materials widely adopted for applications in integrated photonics.

physics.optics↗

Proximity-induced collective modes in an unconventional superconductor heterostructure

Unconventional superconductors have been long sought for their potential applications in quantum technologies and devices. A key challenge impeding this effort is the difficulty associated with probing and characterizing candidate materials and establishing their order parameter. In this Letter, we present a platform that allows us to spectroscopically probe unconventional superconductivity in thin-layer materials via the proximity effect. We show that inducing an s-wave gap in a sample with an intrinsic d-wave instability leads to the formation of bound-states of quasiparticle pairs, which manifest as a collective mode in the d-wave channel. This finding provides a way to study the underlying pairing interactions vicariously through the collective mode spectrum of the system. Upon further cooling of the system we observe that this mode softens considerably and may even condense, signaling the onset of time-reversal symmetry breaking superconductivity. Therefore, our proposal also allows for the creation and study of these elusive unconventional states.

cond-mat.supr-con↗

Transition from Lorentz to Fano Spectral Line Shapes in Non-Relativistic Quantum Electrodynamics

Spectroscopic signatures associated with symmetric Lorentzian and asymmetric Fano line shapes are ubiquitous. Distinct features of Fano resonances in contrast with conventional symmetric resonances have found several applications in photonics such as optical switching, sensing, lasing, and nonlinear and slow-light devices. Therefore, it is important to have control over the generation of these resonances. In this work, we show through ab initio simulations of coupled light-matter systems that Fano interference phenomena can be realized in a multimode photonic environment by strong coupling to the electromagnetic continuum. Specifically, we show that by effectively enhancing the light-matter coupling strength to the photon continuum in an experimentally feasible way, we can achieve a transition from Lorentzian to Fano lines shapes for both electronic and polaritonic excitations. An important outcome of switching between these spectral signatures is the possibility to control the Purcell enhancement of spontaneous emission alongside electromagnetically induced transparency which is a special case of Fano resonances. Switching from Fano back to a Lorentzian profile can be achieved by physically reducing the coupling strength to the continuum of modes. Our results hold potential for realizing tunable Fano resonances of molecules and materials interacting with the electromagnetic continuum within multimode photonic environments.

physics.optics↗

Tunable quantum logic gate on photonic qubits with a ladder emitter

We present a scheme to implement a passive and deterministic controlled-variable phase gate on photonic qubits encoded in the frequency basis. Our gate employs a cascade system with the ground to first excited state interacting with the control photon of a given polarization, and the first to second excited state transition interacting with the target photon of the orthogonal polarization. By controlling the relative detuning between the target photon and the frequency of the transition between the first and second excited states of the cascade emitter, we enable any controlled-phase operation from 0 to $π$. This gate does not utilize any active control and needs only a single cascade emitter, enabling low-footprint and more efficient decomposition of quantum circuits, especially those rooted in the quantum Fourier transform.

quant-ph↗

Axial Higgs Mode Detected by Quantum Pathway Interference in RTe3

The observation of the Higgs boson solidified the standard model of particle physics. However, explanations of anomalies (e.g. dark matter) rely on further symmetry breaking calling for an undiscovered axial Higgs mode. In condensed matter the Higgs was seen in magnetic, superconducting and charge density wave(CDW) systems. Uncovering a low energy mode's vector properties is challenging, requiring going beyond typical spectroscopic or scattering techniques. Here, we discover an axial Higgs mode in the CDW system RTe3 using the interference of quantum pathways. In RTe3 (R=La,Gd), the electronic ordering couples bands of equal or different angular momenta. As such, the Raman scattering tensor associated to the Higgs mode contains both symmetric and antisymmetric components, which can be excited via two distinct, but degenerate pathways. This leads to constructive or destructive interference of these pathways, depending on the choice of the incident and Raman scattered light polarization. The qualitative behavior of the Raman spectra is well-captured by an appropriate tight-binding model including an axial Higgs mode. The elucidation of the antisymmetric component provides direct evidence that the Higgs mode contains an axial vector representation (i.e. a pseudo-angular momentum) and hints the CDW in RTe3 is unconventional. Thus we provide a means for measuring collective modes quantum properties without resorting to extreme experimental conditions.

physics.optics↗

Imaging phonon-mediated hydrodynamic flow in WTe2

In the presence of interactions, electrons in condensed-matter systems can behave hydrodynamically, exhibiting phenomena associated with classical fluids, such as vortices and Poiseuille flow. In most conductors, electron-electron interactions are minimized by screening effects, hindering the search for hydrodynamic materials; however, recently, a class of semimetals has been reported to exhibit prominent interactions. Here we study the current flow in the layered semimetal tungsten ditelluride by imaging the local magnetic field using a nitrogen-vacancy defect in a diamond. We image the spatial current profile within three-dimensional tungsten ditelluride and find that it exhibits non-uniform current density, indicating hydrodynamic flow. Our temperature-resolve current profile measurements reveal a non-monotonic temperature dependence, with the strongest hydrodynamic effects at approximately 20 K. We also report ab initio calculations showing that electron-electron interactions are not explained by the Coulomb interaction alone, but are predominantly mediated by phonons. This provides a promising avenue in the search for hydrodynamic flow and prominent electron interactions in high-carrier-density materials.

cond-mat.mes-hall↗

Capturing Non-Markovian Dynamics on Near-Term Quantum Computers

With the rapid progress in quantum hardware, there has been an increased interest in new quantum algorithms to describe complex many-body systems searching for the still-elusive goal of 'useful quantum advantage'. Surprisingly, quantum algorithms for the treatment of open quantum systems (OQSs) have remained under-explored, in part due to the inherent challenges of mapping non-unitary evolution into the framework of unitary gates. Evolving an open system unitarily necessitates dilation into a new effective system to incorporate critical environmental degrees of freedom. In this context, we present and validate a new quantum algorithm to treat non-Markovian dynamics in OQSs built on the Ensemble of Lindblad's Trajectories approach, invoking the Sz.-Nagy dilation theorem. Here we demonstrate our algorithm on the Jaynes-Cummings model in the strong coupling and detuned regimes, relevant in quantum optics and driven quantum systems studies. This algorithm, a key step towards generalized modeling of non-Markovian dynamics on a noisy-quantum device, captures a broad class of dynamics and opens up a new direction in OQS problems.

quant-ph↗

Heterogeneous Multipartite Entanglement Purification for Size-Constrained Quantum Devices

The entanglement resource required for quantum information processing comes in a variety of forms, from Bell states to multipartite GHZ states or cluster states. Purifying these resources after their imperfect generation is an indispensable step towards using them in quantum architectures. While this challenge, both in the case of Bell pairs and more general multipartite entangled states, is mostly overcome in the presence of perfect local quantum hardware with unconstrained qubit register sizes, devising optimal purification strategies for finite-size realistic noisy hardware has remained elusive. Here we depart from the typical purification paradigm for multipartite states explored in the last twenty years. We present cases where the hardware limitations are taken into account, and surprisingly find that smaller `sacrificial' states, like Bell pairs, can be more useful in the purification of multipartite states than additional copies of these same states. This drastically simplifies the requirements and presents a fundamentally new pathway to leverage near term networked quantum hardware.

quant-ph↗

Implementing a Ternary Decomposition of the Toffoli Gate on Fixed-FrequencyTransmon Qutrits

Quantum computation is conventionally performed using quantum operations acting on two-level quantum bits, or qubits. Qubits in modern quantum computers suffer from inevitable detrimental interactions with the environment that cause errors during computation, with multi-qubit operations often being a primary limitation. Most quantum devices naturally have multiple accessible energy levels beyond the lowest two traditionally used to define a qubit. Qudits offer a larger state space to store and process quantum information, reducing complexity of quantum circuits and improving efficiency of quantum algorithms. Here, we experimentally demonstrate a ternary decomposition of a multi-qubit operation on cloud-enabled fixed-frequency superconducting transmons. Specifically, we realize an order-preserving Toffoli gate consisting of four two-transmon operations, whereas the optimal order-preserving binary decomposition uses eight \texttt{CNOT}s on a linear transmon topology. Both decompositions are benchmarked via truth table fidelity where the ternary approach outperforms on most sets of transmons on \texttt{ibmq\_jakarta}, and is further benchmarked via quantum process tomography on one set of transmons to achieve an average gate fidelity of 78.00\% $\pm$ 1.93\%.

quant-ph↗

Generalized Design Principles for Hydrodynamic Electron Transport in Anisotropic Metals

Interactions of charge carriers with lattice vibrations, or phonons, play a critical role in unconventional electronic transport of metals and semimetals. Recent observations of phonon-mediated collective electron flow in bulk semimetals, termed electron hydrodynamics, present new opportunities in the search for strong electron-electron interactions in high carrier density materials. Here we present the general transport signatures of such a second-order scattering mechanism, along with analytical limits at the Eliashberg level of theory. We study electronic transport, using $ab$ $initio$ calculations, in finite-size channels of semimetallic ZrSiS and TaAs$_2$ with and without topological band crossings, respectively. The order of magnitude separation between momentum-relaxing and momentum-conserving scattering length-scales across a wide temperature range make both of them promising candidates for further experimental observation of electron hydrodynamics. More generally, our calculations show that the hydrodynamic transport regime can be realized in a much broader class of anisotropic metals and does not, to first order, rely on the topological nature of the bands. Finally, we discuss general design principles guiding future search for hydrodynamic candidates, based on the analytical formulation and our $ab$ $initio$ predictions. We find that systems with strong electron-phonon interactions, reduced electronic phase space, and suppressed phonon-phonon scattering at temperatures of interest are likely to feature hydrodynamic electron transport. We predict that layered and/or anisotropic semimetals composed of half-filled $d$-shells and light group V/VI elements with lower crystal symmetry are ideal candidates to observe hydrodynamic phenomena in future.

cond-mat.mtrl-sci↗