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Priyanka Mondal

Publications and source records attributed to Priyanka Mondal.

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Excitonic fingerprints of magnetic configurations and switching in multilayer CrSBr

The coupling between electronic states and magnetism provides a route towards optical readout and control of magnetic information. In the magnetic semiconductor CrSBr, excitons are coupled to magnetic order, making their optical response sensitive to the underlying magnetization. Here, we show that the energy and oscillator strength of bulk and surface excitons provide distinct spectroscopic fingerprints of magnetic configurations and switching pathways. We distinguish domain-wall-mediated magnetization reversal, manifested by continuous spectral evolution as a domain wall traverses the optical spot, from abrupt, large-area magnetization reversal. Using the resulting excitonic fingerprints, we reconstruct successive magnetic configurations in 4- and 5-layer CrSBr during the transition from ferromagnetic to antiferromagnetic order. We further find that the sensitivity to magnetic order is strongly exciton-dependent: low-energy excitons resolve intermediate and surface-related configurations, whereas a higher-energy exciton predominantly exhibits a transfer of oscillator strength between ferromagnetic and antiferromagnetic resonances. These results establish excitonic spectroscopy as a sensitive probe of layer-dependent magnetic configurations and their switching pathways in layered magnetic semiconductors.

cond-mat.mtrl-sci

Detecting Magnetic Phase Transitions in Ion-Irradiated CrSBr Through Resonant Raman Scattering

Controlling magnetic phases and accurately determining their transition temperatures are essential for the development of low-dimensional magnetic materials. Here, we demonstrate that He$^+$ ion irradiation provides a versatile route for engineering magnetic phases in layered CrSBr and establish temperature-dependent polarization-resolved Raman spectroscopy as a sensitive optical probe for identifying irradiation-induced magnetic phase transitions. We reveal that the magnetic response of the modified CrSBr is governed by both irradiation dose and crystal thickness. The temperature evolution of the Raman tensor elements resolves the antiferromagnetic transition in pristine CrSBr at T$_N \approx 132$ K as well as irradiation-induced magnetic transitions at T$_C \approx 105-110$ K and T$_D \approx 40$ K corresponding to ferromagnetic and defect-related magnetic phase transitions. Complementary magneto-optical measurements confirm the progressive suppression of antiferromagnetic order and the emergence of new defect-engineered magnetic phases, including pure ferromagnetic behavior at high irradiation doses. These findings establish irradiated CrSBr as a platform for controllable magnetic phase engineering while demonstrating polarization-resolved Raman spectroscopy as a rapid, non-destructive, and broadly applicable method for probing magnetic phase transitions in van der Waals magnets.

cond-mat.mtrl-sci

Twist-tuned exchange and hysteresis in a bilayer van der Waals magnet

Moiré superlattices in twisted bilayers enable profound reconstructions of the electronic bandstructure, giving rise to correlated states with remarkable tunability. Extending this paradigm to van der Waals magnets, twisting creates spatially varying interlayer exchange interactions that stabilize emergent spin textures and the coexistence of ferromagnetic and antiferromagnetic domains. Here, we demonstrate the emergence of robust magnetic hysteresis in bilayer CrSBr upon twisting by an angle of ~ 3°. This is observed as the corresponding hysteretic evolution of the exciton energy, that directly correlates with the bilayer magnetic state, in magnetic field dependent photoluminescence measurements. A two-sublattice model captures this behavior, attributing it to the twist-induced reduction of interlayer exchange that stabilizes both parallel and antiparallel spin configurations across a broad field range. Comparison with experiment enables quantitative extraction of the effective exchange strength. Remarkably, the system exhibits coherent averaging across the moiré supercell, yielding an effective monodomain response characterized by switching into the antiferromagnetic state, rather than forming spin textures or fragmented domains. Spatially resolved measurements further uncover local variations in hysteresis loops, consistent with position-dependent modulation of the average exchange interaction. Our results establish twist engineering as a powerful route to programmable magnetic memories in two-dimensional magnets, harnessing the robustness of antiferromagnetic order.

cond-mat.mtrl-sci

Interplay of vibrational, electronic, and magnetic states in CrSBr

The van der Waals antiferromagnet CrSBr exhibits coupling of vibrational, electronic, and magnetic degrees of freedom, giving rise to distinctive quasi-particle interactions. We investigate these interactions across a wide temperature range using polarization-resolved Raman spectroscopy at various excitation energies, complemented by optical absorption and photoluminescence excitation (PLE) spectroscopy. Under 1.96 eV excitation, we observe pronounced changes in the A$_g^1$, A$_g^2$, and A$_g^3$ Raman modes near the Néel temperature, coinciding with modifications in the oscillator strength of excitonic transitions and clear resonances in PLE. The distinct temperature evolution of Raman tensor elements and polarization anisotropy for Raman modes indicates that they couple to different excitonic and electronic states. The suppression of the excitonic state's oscillation strength above the Néel temperature could be related to the magnetic phase transition, thereby connecting these excitonic states and Raman modes to a specific spin alignment. These observations make CrSBr a versatile platform for probing quasi-particle interactions in low-dimensional magnets and provide insights for applications in quantum sensing and quantum communication.

cond-mat.mtrl-sci

Magnetic Correlation Spectroscopy in CrSBr

CrSBr is an air-stable magnetic van der Waals semiconductor with strong magnetic anisotropy, where the interaction of excitons with the magnetic order enables the optical identification of different magnetic phases. Here, we study the magnetic anisotropy of multi-layer CrSBr inside a three-axis vector magnet and correlate magnetic order and optical transitions in emission and absorption. We identify layer by layer switching of the magnetization through drastic changes of the optical emission and absorption energy and strength as a function of the applied magnetic field. We correlate optical transitions in reflection spectra with photoluminescence (PL) emission using a transfer-matrix analysis and find that ferromagnetic and antiferromagnetic order between layers can coexist in the same crystal. In the multi-peak PL emission the intensity of energetically lower lying transitions reduces monotonously with increasing field strength whereas energetically higher lying transitions around the bright exciton $X_B$ brighten close to the saturation field. Using this contrasting behavior we can therefore correlate transitions with each other.

cond-mat.mtrl-sci

Raman Polarization Switching in CrSBr

Semiconducting CrSBr is a layered A-type antiferromagnet, with individual layers antiferromagnetically coupled along the stacking direction. Due to its unique orthorhombic crystal structure, CrSBr exhibits highly anisotropic mechanical and optoelectronic properties acting itself as a quasi-1D material. CrSBr demonstrates complex coupling phenomena involving phonons, excitons, magnons, and polaritons. Here we show through polarization-resolved resonant Raman scattering the intricate interaction between the vibrational and electronic properties of CrSBr. For samples spanning from few-layer to bulk thickness, we observe that the polarization of the A$_g^2$ Raman mode can be rotated by 90 degrees, shifting from alignment with the crystallographic a (intermediate magnetic) axis to the b (easy magnetic) axis, depending on the excitation energy. In contrast, the A$_g^1$ and A$_g^3$ modes consistently remain polarized along the b axis, regardless of the laser energy used. We access real and imaginary parts of the Raman tensor in our analysis, uncovering resonant electron-phonon coupling.

cond-mat.mtrl-sci

Electrically Controlled Interfacial Charge Transfer Induced Excitons in MoSe2-WSe2 Lateral Heterostructure

Controlling excitons and their transport in two-dimensional (2D) transition metal dichalcogenides (TMDs) heterostructures is central to advancing photonics and electronics on-chip integration. We investigate the controlled generation and manipulation of excitons and their complexes in monolayer (1L) MoSe2-WSe2 lateral heterostructure (LHS), directly grown via water-assisted chemical vapor deposition. Using a field-effect transistor design by incorporating a few-layer graphene back gate, single-layer graphene edge contact and encapsulation with few-layer hexagonal boron nitride, we achieve precise electrical tuning of exciton complexes and their transfer across 1D interfaces. At cryogenic temperatures (4 K), photoluminescence and photocurrent maps reveal the synergistic effect of local electric field and interface phenomena in the modulation of excitons, trions, and free carriers. We observe spatial variations in exciton and trion densities driven by exciton-trion conversion under electrical manipulation. The first-principle density functional theory calculation reveals significant band modification at the lateral interfaces and graphene-TMDs contact region. Furthermore, we demonstrate the versatility of 2D TMDS LHS in hosting and manipulating quantum emitters, achieving precise control over narrow-band emissions through modulating carrier injection and electrical biasing. This work extends the boundary of the present understanding of excitonic behaviour within lateral heterojunctions, highlighting the potential for controlled exciton manipulation across 1D interfaces and paving the way for next-generation electro-optical quantum devices.

cond-mat.mes-hall

Applying consensus and replication securely with FLAQR

Availability is crucial to the security of distributed systems, but guaranteeing availability is hard, especially when participants in the system may act maliciously. Quorum replication protocols provide both integrity and availability: data and computation is replicated at multiple independent hosts, and a quorum of these hosts must agree on the output of all operations applied to the data. Unfortunately, these protocols have high overhead and can be difficult to calibrate for a specific application's needs. Ideally, developers could use high-level abstractions for consensus and replication to write fault-tolerant code by that is secure by construction. This paper presents Flow-Limited Authorization for Quorum Replication (FLAQR), a core calculus for building distributed applications with heterogeneous quorum replication protocols while enforcing end-to-end information security. Our type system ensures that well-typed FLAQR programs cannot_fail_ (experience an unrecoverable error) in ways that violate their type-level specifications. We present noninterference theorems that characterize FLAQR's confidentiality, integrity, and availability in the presence of consensus, replication, and failures, as well as a liveness theorem for the class of majority quorum protocols under a bounded number of faults.

cs.PL

When can localized spins interacting with conduction electrons in ferro- or antiferromagnets be described classically via the Landau-Lifshitz equation: Transition from quantum many-body entangled to quantum-classical nonequilibrium states

Experiments in spintronics and magnonics operate with macroscopically large number of localized spins within ferromagnetic (F) or antiferromagnetic (AF) materials, so that their nonequilibrium dynamics is standardly described by the Landau-Lifshitz (LL) equation treating localized spins as classical vectors of fixed length. However, spin is a genuine quantum degree of freedom, and even though quantum effects become progressively less important for spin value $S>1$, they exist for all $S < \infty$. While this has motivated exploration of limitations/breakdown of the LL equation, by using examples of F insulators, analogous comparison of fully quantum many-body vs. quantum (for electrons)-classical (for localized spins) dynamics in systems where nonequilibrium conduction electrons are present is lacking. Here we employ quantum Heisenberg F or AF chains of $N=4$ sites, whose localized spins interact with conduction electrons via $sd$ exchange interaction, to perform such comparison by starting from unentangled pure (at zero temperature) or mixed (at finite temperature) quantum state of localized spins as the initial condition. This reveals that quantum-classical dynamics can faithfully reproduce fully quantum dynamics in the F metallic case, but only when spin $S$, Heisenberg exchange between localized spins and $sd$ exchange are sufficiently small. Increasing any of these three parameters can lead to substantial deviations, which are explained by the dynamical buildup of entanglement between localized spins and/or between them and electrons. In the AF metallic case, substantial deviations appear even at early times, despite starting from unentangled Néel state, which therefore poses a challenge on how to rigorously justify wide usage of the LL equation in phenomenological modeling of antiferromagnetic spintronics experiments.

cond-mat.str-el

Spintronics meets density matrix renormalization group: Quantum spin torque driven nonclassical magnetization reversal and dynamical buildup of long-range entanglement

We introduce time-dependent density matrix renormalization group (tDMRG) as a solution to long standing problem in spintronics -- how to describe spin-transfer torque (STT) between flowing spins of conduction electrons and localized spins within a magnetic material by treating the dynamics of both spin species fully quantum-mechanically. In contrast to conventional Slonczewski-Berger STT, where the localized spins are viewed as classical vectors obeying the Landau-Lifshitz-Gilbert equation and where their STT-driven dynamics is initiated only when the spin-polarization of flowing electrons and localized spins are noncollinear, quantum STT can occur when these vectors are collinear but antiparallel. Using tDMRG, we simulate the time evolution of a many-body quantum state of electrons and localized spins, where the former are injected as a spin-polarized current pulse while the latter comprise a quantum Heisenberg ferromagnetic metallic (FM) spin-$\frac{1}{2}$ XXZ chain initially in the ground state with spin-polarization antiparallel to that of injected electrons. The quantum STT reverses the direction of localized spins, but without rotation from the initial orientation, when the number of injected electrons exceeds the number of localized spins. Such nonclassical reversal, which is absent from LLG dynamics, is strikingly inhomogeneous across the FM chain and it can be accompanied by reduction of the magnetization associated with localized spins, even to zero at specific locations. This is because quantum STT generates a highly entangled nonequilibrium many-body state of all flowing and localized spins, despite starting from the initially unentangled ground state of a mundane FM. Furthermore, the mutual information between localized spins at the FM edges remains nonzero even at infinite separation as the signature of dynamical buildup of long-range entanglement.

cond-mat.str-el

Quantum spin torque driven transmutation of antiferromagnetic Mott insulator

The standard model of spin-transfer torque (STT) in antiferromagnetic spintronics considers exchange of angular momentum between quantum spins of flowing electrons and noncollinear-to-them localized spins treated as classical vectors. These vectors are assumed to realize Néel order in equilibrium, $\uparrow \downarrow \ldots \uparrow \downarrow$, and their STT-driven dynamics is described by the Landau-Lifshitz-Gilbert (LLG) equation. However, many experimentally employed materials (such as archetypal NiO) are strongly electron-correlated antiferromagnetic Mott insulators (AFMI) where localized spins form a ground state quite different from the unentangled Néel state $|\!\! \uparrow \downarrow \ldots \uparrow \downarrow \rangle$. The true ground state is entangled by quantum spin fluctuations, leading to expectation value of all localized spins being zero, so that LLG dynamics of classical vectors of fixed length rotating due to STT cannot even be initiated. Instead, a fully quantum treatment of both conduction electrons and localized spins is necessary to capture exchange of spin angular momentum between them, denoted as quantum STT. We use a recently developed time-dependent density matrix renormalization group approach to quantum STT to predict how injection of a spin-polarized current pulse into a normal metal layer coupled to AFMI overlayer via exchange interaction and possibly small interlayer hopping -- which mimics, e.g., topological-insulator/NiO bilayer employed experimentally -- will induce nonzero expectation value of AFMI localized spins. This new nonequilibrium phase is a spatially inhomogeneous ferromagnet with zigzag profile of localized spins. The total spin absorbed by AFMI increases with electron-electron repulsion in AFMI, as well as when the two layers do not exchange any charge.

cond-mat.str-el

Quantum spin-transfer torque induced nonclassical magnetization dynamics and electron-magnetization entanglement

The standard spin-transfer torque (STT)---where spin-polarized current drives dynamics of magnetization viewed as a classical vector---requires noncollinearity between electron spins carried by the current and magnetization of a ferromagnetic layer. However, recent experiments [A. Zholud et al., Phys. Rev. Lett. 119, 257201 (2017)] observing magnetization dynamics in spin valves at cryogenic temperatures, even when electron spin is collinear to magnetization, point at overlooked quantum effects in STT which can lead to highly nonclassical magnetization states. Using fully quantum many-body treatment, where an electron injected as spin-polarized wave packet interacts with local spins comprising the anisotropic quantum Heisenberg ferromagnetic chain, we define quantum STT as any time evolution of local spins due to initial many-body state not being an eigenstate of electron+local-spins system. For time evolution caused by injected spin-down electron scattering off local up-spins, entanglement between electron subsystem and local spins subsystem takes place leading to decoherence and, therefore, shrinking of the total magnetization but without rotation from its initial orientation which explains the experiments. Furthermore, the same processes---entanglement and thereby induced decoherence---are present also in standard noncollinear geometry, together with the usual magnetization rotation. This is because STT in quantum many-body picture is caused only by electron spin-down factor state, and the only difference between collinear and noncollinear geometries is in relative size of the contribution of initial many-body state containing such factor state to superpositions of separable many-body quantum states generated during time evolution.

cond-mat.str-el