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Sangeeta Sharma

Publications and source records attributed to Sangeeta Sharma.

At least 19 recordsLinked to original sources

All optical ultrafast pure spin current in the altermagnet Cr$_2$SO

All-optical generation of pure spin current -- the flow of spin in the absence of a corresponding charge flow -- relies on a symmetry based compensation of valley charge. The 2d $d$-wave altermagnets, ideal spintronics materials due to a very low spin-orbit coupling, possess a magnetic point group and highly anisotropic valley manifolds that would appear to preclude such current compensation, excluding them as materials for the ultrafast generation of pure spin current. Here we show that infra-red valley excitation combined with a THz pulse envelope allows the generation of large and nearly 100\% pure spin currents in the altermagnet Cr$_2$SO. Our approach is based on a valley selection rule coupling linearly polarized light to spin opposite valleys, along with the intrinsic momentum shift that a co-occurring THz pulse imbues a valley spin excitation with. These results thus provide a practical and all-optical route to the generation of pure spin current in $d$-wave 2d altermagnets, opening a route to lightwave control of spin in an environment with very low intrinsic spin mixing.

cond-mat.mtrl-sci

Ultrafast ghost Hall states in a 2d altermagnet

Two-dimensional materials that exhibit optically active spin and valley degrees of freedom represent one of the most fascinating -- and potentially most technologically useful -- platforms for the ultrafast interaction of light and matter. Here we show, via the example of Cr$_2$SO, that two dimensional altermagnets host valley states controllable by femtosecond laser light: linearly polarized light pulses excite charge at one of two inequivalent valleys, with which valley charge is excited at determined by the polarization vector direction. This underpins a rich spin and valley physics including: (i) valleytronics $-$ the generation of nearly 100$\%$ spin polarized valley currents, as well as (ii) a "ghost Hall" effect $-$ the ultrafast creation of states in which spin and charge currents are orthogonal without invoking Hall physics. Our findings establish 2d altermagents as a platform providing a new route for the control of spin- and charge currents at ultrafast times.

cond-mat.mes-hall

Ultrafast N\'eel vector switching

We predict ultrafast switching in a chiral anti-ferromagnet that occurs at femtosecond times, nearly 5 orders of magnitude faster than the torque induced nanosecond switching previously observed. The physical mechanism, quite different from that which drives slow switching, involves the creation of massive effective magnetic fields by ultrafast spin current injection. Identifying these fields as key to femtosecond rotation, we establish simple practical rules for their maximisation with wide applicability to all magnetised materials. Employing state-of-the-art time-dependent density-functional theory and using the example of chiral magnet, Mn$_3$Sn, we induce ultrafast rotation enough to drive the switching of magnetic order between the six possible non-collinear ground states. We further demonstrate the possibility of undoing this switching by subsequent injection of oppositely polarized spin current. Our findings place chiral anti-ferromagnets as a materials platform for femtosecond N\'eel-vector switching, opening a route towards the manipulation of magnetic matter at ultrafast times.

cond-mat.mtrl-sci

Valley polarization of graphene via the saddle point

Graphene, and other members of the monolayer Xene family, represent an ideal materials platform for "valleytronics", the control of valley localized charge excitations. The absence of a gap in these semi-metals, however, precludes valley excitation by circularly polarized light pulses, sharply circumscribing the possibility of a lightwave valleytronics in these materials. Here we show that combining a deep ultraviolet linearly polarized light pulse with a THz envelope can induce highly valley polarized states in graphene. This dual frequency lightform operates by (i) the deep ultraviolet pulse activating a selection rule at the M saddle points and (ii) the THz pulse displacing the M point excitation to one of the low-energy K valleys. Employing both tight-binding and state-of-the-art time dependent density functional theory, we show that such a pulse results in a near perfect valley polarized excitation in graphene, thus providing a route via the saddle point to a lightwave valleytronics in the gapless Xene family.

physics.optics

Generation of pure, spin polarized, and unpolarized charge currents at the few cycle limit of circularly polarized light

In certain members of the transition metal dichalcogenide (TMDC) family, laser pulses of oppositely circularly polarized light excite electrons of opposite spin. Here we show that in the few cycle limit such pulses generate not only a spin density excitation, but also a spin current excitation. Employing the example of the TMDC WSe$_2$ we show that pure spin currents, the flow of spin in the absence of net charge flow, 100% spin polarized currents, and charge currents are all accessible and controllable by tuning the amplitude of ~ 5 femtosecond gap tuned light pulses. Underpinning this physics is a symmetry lowering of the valley charge excitation from C3 at long duration to C2 in the few cycle limit, imbuing the excitation with net current. Our results both highlight the emergence of a rich light-spin current coupling at ultrafast times in the TMDC family, as well presenting a route to the all-optical generation of pure spin currents.

cond-mat.mes-hall

Ultrafast controlling net magnetization in g-wave altermagnets via laser fields

The diverse nodal spin structures in d/g/i-wave altermagnets (AM) may cause distinct light-induced spin responses yet remain poorly understood. Using time-dependent density functional theory (TDDFT), we reveal that laser induced ultrafast demagnetization dynamics in the g-wave AM CrSb are strongly governed by the laser incidence direction. Under normal incidence along the [0001] axis, two Cr sublattices exhibit symmetric temporal demagnetization but with different amplitudes, preserving the net-zero magnetization, unlike the behavior in d-wave AM. Off-normal incidence, however, induces pronounced asymmetric demagnetization between sublattices, transiently driving the system into a ferrimagnetic-like state with a sizable net magnetization. This direction-dependent response arises from the characteristic nodal structures in bulk g-wave AM electronic structure, which enable anisotropic optical intersite spin transfer (OISTR). By comparing g-wave and d-wave AMs, we propose that light-induced magnetization arises when laser polarization aligns with spin-uncompensated regions in electronic structures. This can be readily determined from the local spin density of states along specific band paths. Our results provide a fundamental understanding for laser-induced ultrafast dynamics in AM.

cond-mat.mtrl-sci

Tunable magnons in a dual-gated 2D antiferromagnet

The layered antiferromagnet CrSBr features magnons coupled to other quasiparticles, including excitons and polaritons, enabling their easy optical accessibility. In this work, we investigate the tunability of magnons in few-layered devices in response to changes in carrier density and the application of a perpendicular electric field. We demonstrate an on-chip tunability of the in- and out-of-phase magnon frequencies by up to 2 GHz. While the frequencies of both modes increase with the electron density, we observe an asymmetric response with respect to the electric field in a dual-gated trilayer device. To understand the mechanism of this disparity, we develop a layer-resolved macrospin model describing the magnetic dynamics in thin, non-uniformly doped devices. Through this model we establish the doping- and electric-field-dependence of the exchange interaction, magnetic anisotropy, and magnetic moment of individual layers. Our results advance the applications of gate-tunable magnonic devices based on 2D materials.

cond-mat.mes-hall

Accelerated ultrafast demagnetization of an interlayer-exchange-coupled Co/Mn/Co trilayer

We investigate the ultrafast magnetization dynamics of an interlayer-exchange-coupled Co/Mn/Co trilayer system after excitation with an ultrafast optical pump. We probe element- and time-resolved ferromagnetic order by X-ray magnetic circular dichroism in resonant reflectivity. We observe an accelerated Co demagnetization time in the case of weak total parallel interlayer coupling at 9.5 ML Mn thickness for antiparallel alignment of both Co layers compared to parallel alignment as well as for parallel alignment in the case of strong parallel interlayer coupling at 11 ML of Mn. From ab initio time-dependent density functional theory calculations, we conclude that optically induced intersite spin transfer of spin-polarized electrons from Co into Mn acts as a decay channel to enhance and accelerate ultrafast demagnetization. This spin transfer can only take place in case of a collinear Mn spin structure. We argue that this is the case for antiparallel alignment of both Co layers at 9.5 ML Mn thickness and parallel alignment in case of 11 ML of Mn. Our results point out that an antiferromagnetic spacer layer and its spin structure have a significant effect on the magnetization dynamics of adjacent ferromagnetic layers. Our findings provide further insight into fundamental mechanisms of ultrafast demagnetization and may lead to improve dynamics in multilayered systems for faster optical switching of magnetic order.

cond-mat.mtrl-sci

Coupled femto-excitons, free carriers and light

Non-equilibrium quantum matter generated by ultrafast laser light opens new pathways in fundamental condensed matter physics, as well as offering rich control possibilities in "tailoring matter by light". Here we explore the coupling between free carriers and excitons mediated by femtosecond scale laser pulses. Employing monolayer WSe$_2$ and an {\it ab-initio} treatment of pump-probe spectroscopy we find that, counter-intuitively, laser light resonant with the exciton can generate massive enhancement of the early time free carrier population. This exhibits complex dynamical correlation to the excitons, with an oscillatory coupling between free carrier population and exciton peak height that persists. Our results both unveil "femto-excitons" as possessing a rich femtosecond dynamics as well as, we argue, allowing tailoring of early time light-matter interaction via laser pulse design to control simultaneously excitonic and free carrier physics at ultrafast times.

cond-mat.mtrl-sci

Ultrafast Saddletronics

Low energy valleys in the band structure of 2d materials represent a potential route to the ultrafast writing of information in quantum matter by laser light, with excited charge at the K or K$^\ast$ valleys representing the fundamental states of 1 and 0. Here we demonstrate that a second electronic feature, the saddle point, is endowed with lightwave control over information states. Linearly polarized light is shown to excite 2 of the 3 inequivalent M point saddles in graphene, generating three possible excited configurations, with which of these are realised determined by the polarization vector direction. We show that saddle excitation is highly robust, with "saddle polarized" states created both in the sub-cycle strong field regime and the long time limit of extended multi-cycle pulses. Our findings, applicable to other members of the graphene family and Xenes such as stanene, point towards a rich and ultrafast light based manipulation of matter based on the saddle point.

cond-mat.mes-hall

Giant moment increase by ultrafast laser light

It is now well established that a few femtosecond laser pulse will induce an ultrafast loss of moment in a magnetic material. Here we show that the opposite effect can also occur: an ultrafast increase in moment. Employing both tight-binding and state-of-the-art time dependent density functional theory we find that laser light tuned to the majority spin conduction band in the 2d magnets CrI$_3$ and CrSBr generates an ultrafast giant moment increase, of up to 33\% in the case of CrI$_3$ (2~$μ_B$). Underpinning this is spin-orbit induced valence band spin texture that, in combination with a strong field light pulse, facilitates an optical spin flip transition involving both intra- and inter-band excitation. Our findings, that establish a general mechanism by which ultrafast light pulses may enhance as well as decrease the magnetic moment, point towards rich possibilities for light control over magnetic matter at femtosecond times.

cond-mat.mtrl-sci

Magnetizing altermagnets by ultrafast asymmetric spin dynamics

Laser pulses are known to induce symmetric demagnetization: equal loss of magnetic moments in the identical sublattices of antiferromagnets and ferromagnets at ultrashort timescales. Using time-dependent density functional theory, we show that linearly polarized laser pulses can drive asymmetric demagnetization between otherwise identical sublattices in the $d$-wave compensated altermagnet (AM) RuO$_2$, resulting in a \textit{photo-induced ferrimagnetic state} with a strong net magnetization of $\sim$0.2 $\mu_B$ per unit cell. The sign and magnitude of this metastable magnetization are highly controllable by laser polarization. We identify polarization-selective asymmetric optical intersite spin transfer (a-OISTR) as the primary mechanism generating the net moment, followed by asymmetric spin flips (a-SF) that further amplifies it. Both effects originate from the characteristic nodal spin band topology of \textit{d}-wave AMs. Moreover, we demonstrate that this laser-induced magnetization is universal across various $d$-wave AMs, including experimentally confirmed KV$_2$Se$_2$O and RbV$_2$Te$_2$O. We uncover a robust route to light-controlled magnetization in AMs on ultrafast timescales.

cond-mat.mtrl-sci

The 2025 Roadmap to Ultrafast Dynamics: Frontiers of Theoretical and Computational Modelling

The exploration of ultrafast phenomena is a frontier of condensed matter research, where the interplay of theory, computation, and experiment is unveiling new opportunities for understanding and engineering quantum materials. With the advent of advanced experimental techniques and computational tools, it has become possible to probe and manipulate nonequilibrium processes at unprecedented temporal and spatial resolutions, providing insights into the dynamical behavior of matter under extreme conditions. These capabilities have the potential to revolutionize fields ranging from optoelectronics and quantum information to catalysis and energy storage. This Roadmap captures the collective progress and vision of leading researchers, addressing challenges and opportunities across key areas of ultrafast science. Contributions in this Roadmap span the development of ab initio methods for time-resolved spectroscopy, the dynamics of driven correlated systems, the engineering of materials in optical cavities, and the adoption of FAIR principles for data sharing and analysis. Together, these efforts highlight the interdisciplinary nature of ultrafast research and its reliance on cutting-edge methodologies, including quantum electrodynamical density-functional theory, correlated electronic structure methods, nonequilibrium Green's function approaches, quantum and ab initio simulations.

cond-mat.mtrl-sci

Creation and control of valley currents in graphene by few cycle light pulses

Well established for the visible spectrum gaps of the transition metal dichalcogenide family, valleytronics - the control of valley charge and current by light - is comparatively unexplored for the THz gaps that characterize graphene and topological insulators. Here we show that few cycle pulses of THz light can create and control a 100% valley polarized current in graphene, with light wave control over the current magnitude and direction. The latter is equal to an emergent pulse property of few cycle circularly polarized pulses, the "global" carrier envelope phase. Our findings both highlight the richness of few cycle light pulses in control over quantum matter, and provide a route towards a "THz valleytronics" in meV gapped systems.

cond-mat.mes-hall

Ultrafast all-optical generation of pure spin and valley currents

Pure currents comprise the flow of a two state quantum freedom -- for example the electron spin -- in the absence of charge flow. Radically different from the charge currents that underpin present day electronics, in two dimensional materials possessing additional two state freedoms such as valley index they offer profound possibilities for miniaturization and energy efficiency in a next generation spin- and valley- tronics. Here we demonstrate a robust multi-pump light wave protocol capable of generating both pure spin and valley currents on femtosecond times. The generation time is determined by the 2d material gap, with the creation of pure spin current in WSe2 at 40 fs and pure valley current in bilayer graphene at ~200 fs. Our all-optical approach demands no special material design, requiring only a gapped valley active material, and is thus applicable to a wide range of 2d materials.

cond-mat.mes-hall

Optically Induced Ferromagnetic Order in a Ferrimagnet

The parallel or antiparallel arrangement of electron spins plays a pivotal role in determining the properties of a physical system. To meet the demands for innovative technological solutions, extensive efforts have been dedicated to exploring effective methods for controlling and manipulating this arrangement [1]. Among various techniques, ultrashort laser pulses have emerged as an exceptionally efficient tool to influence magnetic order. Ultrafast suppression of the magnetic order [2,3], all-optical magnetization switching [4, 5, 6, 7], and light-induced magnetic phase transitions [8] are just a few notable examples. However, the transient nature of light-induced changes in the magnetic state has been a significant limitation, hindering their practical implementation. In this study, we demonstrate that infrared ultrashort laser pulses can induce a ferromagnetic arrangement of magnetic moments in an amorphous TbCo alloy, a material that exhibits ferrimagnetism under equilibrium conditions. Strikingly, the observed changes in the magnetic properties persist for significantly longer durations than any previously reported findings. Our results reveal that ultrashort optical pulses can generate materials with identical chemical composition and structural state but entirely distinct magnetic arrangements, leading to unique magnetic properties. This breakthrough discovery marks a new era in light-driven control of matter, offering the exciting potential to create materials with properties that were once considered unattainable.

cond-mat.mtrl-sci

How closely does transient magnetic linear dichroism follow the spin moment?

In highly out-of-equilibrium states of matter, such as those induced by a pump laser, the applicability of well established spectroscopic probes of magnetic order are called into question. Here we address the validity of x-ray absorption techniques in pump laser conditions, focusing on magnetic linear dichroism (MLD), a crucial probe of antiferromagnetic (AFM) order. We directly compute the dynamics of the square of the spin moment and compare to those obtained via the MLD response. For AFM FePd the agreement between these distinct routes to the magnetic moment severely degrades at pulse fluences greater than 1 mJ/cm$^2$, indicating a breakdown of the MLD response as an accurate probe of the transient moment. This contrasts with the MLD for ferromagnetic FePt which reliably tracks the moment for fluences (and absorbed energies) up to an order of magnitude greater than the breakdown threshold for AFM FePd. The underlying microscopic reason for this we find to be increased laser induced excitations out of the $d$-band in AFM FePd, where this increase is made possible by the AFM pseudogap.

cond-mat.mtrl-sci

Verification of ultrafast spin transfer effects in FeNi alloys

The optical intersite spin transfer (OISTR) effect was recently verified in Fe$_{50}$Ni$_{50}$ using magneto-optical Kerr measurements in the extreme ultraviolet range. However, one of the main experimental signatures analyzed in this work, namely a magnetic moment increase at a specific energy in Ni, was subsequently found also in pure Ni, where no transfer from one element to another is possible. Hence, it is a much-discussed issue whether OISTR in FeNi alloys is real and whether it can be verified experimentally or not. Here, we present a comparative study of spin transfer in Fe$_{50}$Ni$_{50}$, Fe$_{19}$Ni$_{81}$ and pure Ni. We conclusively show that an increase in the magneto-optical signal is indeed insufficient to verify OISTR. However, we also show how an extended data analysis overcomes this problem and allows to unambiguously identify spin transfer effects. Concomitantly, our work solves the long-standing riddle about the origin of delayed demagnetization behavior of Ni in FeNi alloys.

cond-mat.mtrl-sci