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44
result(s) for
"Prasankumar, R. P."
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Coherent helicity-dependent spin-phonon oscillations in the ferromagnetic van der Waals crystal CrI3
by
Gilinsky, S.
,
Singamaneni, S. R.
,
Paramekanti, A.
in
140/125
,
639/766/119/2793
,
639/766/119/997
2022
The discovery of two-dimensional systems hosting intrinsic magnetic order represents a seminal addition to the rich landscape of van der Waals materials. CrI
3
is an archetypal example, where the interdependence of structure and magnetism, along with strong light-matter interactions, provides a new platform to explore the optical control of magnetic and vibrational degrees of freedom at the nanoscale. However, the nature of magneto-structural coupling on its intrinsic ultrafast timescale remains a crucial open question. Here, we probe magnetic and vibrational dynamics in bulk CrI
3
using ultrafast optical spectroscopy, revealing spin-flip scattering-driven demagnetization and strong transient exchange-mediated interactions between lattice vibrations and spin oscillations. The latter yields a coherent spin-coupled phonon mode that is highly sensitive to the driving pulse’s helicity in the magnetically ordered phase. Our results elucidate the nature of ultrafast spin-lattice coupling in CrI
3
and highlight its potential for applications requiring high-speed control of magnetism at the nanoscale.
CrI3 is a van der Waals material which exhibits magnetic ordering down to the monolayer limit. Here, using ultrafast optical spectroscopy, Padmanabhan and Buessen et al. investigate the coupling between the magnetically ordered spins and lattice distortions, finding a coherent spin-coupled phonon mode.
Journal Article
Temperature-tunable Fano resonance induced by strong coupling between Weyl fermions and phonons in TaAs
2017
Strong coupling between discrete phonon and continuous electron–hole pair excitations can induce a pronounced asymmetry in the phonon line shape, known as the Fano resonance. This effect has been observed in various systems. Here we reveal explicit evidence for strong coupling between an infrared-active phonon and electronic transitions near the Weyl points through the observation of a Fano resonance in the Weyl semimetal TaAs. The resulting asymmetry in the phonon line shape, conspicuous at low temperatures, diminishes continuously with increasing temperature. This behaviour originates from the suppression of electronic transitions near the Weyl points due to the decreasing occupation of electronic states below the Fermi level (
E
F
) with increasing temperature, as well as Pauli blocking caused by thermally excited electrons above
E
F
. Our findings not only elucidate the mechanism governing the tunable Fano resonance but also open a route for exploring exotic physical phenomena through phonon properties in Weyl semimetals.
The study of lattice vibrations coupled to electronic excitations may provide an avenue for exploring exotic physical phenomena. Here, Xu
et al
. observe a Fano resonance in the Weyl semimetal TaAs, revealing evidence for a strong coupling between phonons and Weyl fermions.
Journal Article
Using ultrashort optical pulses to couple ferroelectric and ferromagnetic order in an oxide heterostructure
by
Trugman, S. A.
,
Taylor, A. J.
,
Jia, Q. X.
in
639/301/119/2793
,
639/301/119/996
,
Ferroelectrics
2014
A new approach to all-optical detection and control of the coupling between electric and magnetic order on ultrafast timescales is achieved using time-resolved second-harmonic generation (SHG) to study a ferroelectric (FE)/ferromagnet (FM) oxide heterostructure. We use femtosecond optical pulses to modify the spin alignment in a Ba
0.1
Sr
0.9
TiO
3
(BSTO)/La
0.7
Ca
0.3
MnO
3
(LCMO) heterostructure and selectively probe the ferroelectric response using SHG. In this heterostructure, the pump pulses photoexcite non-equilibrium quasiparticles in LCMO, which rapidly interact with phonons before undergoing spin–lattice relaxation on a timescale of tens of picoseconds. This reduces the spin–spin correlations in LCMO, applying stress on BSTO through magnetostriction. This then modifies the FE polarization through the piezoelectric effect, on a timescale much faster than laser-induced heat diffusion from LCMO to BSTO. We have thus demonstrated an ultrafast indirect magnetoelectric effect in a FE/FM heterostructure mediated through elastic coupling, with a timescale primarily governed by spin–lattice relaxation in the FM layer.
The interaction between ferroelectricity and magnetism is of interest for the use in magnetic information storage devices. Here, the authors achieve the coupling of ferroelectric and ferromagnetic order in an oxide heterostructure by ultrashort optical pulses, offering the optical control of these effects.
Journal Article
Shaking up topology with light
2021
A light-induced topological phase transition is realized in the Dirac semimetal ZrTe
5
by coherently driving symmetry-breaking phonons.
Journal Article
Photocurrent-driven transient symmetry breaking in the Weyl semimetal TaAs
by
Teitelbaum, S. W.
,
Padmanabhan, P.
,
Yang, R.
in
639/301/1019/385
,
639/766/119/2792
,
Biomaterials
2022
Symmetry plays a central role in conventional and topological phases of matter, making the ability to optically drive symmetry changes a critical step in developing future technologies that rely on such control. Topological materials, like topological semimetals, are particularly sensitive to a breaking or restoring of time-reversal and crystalline symmetries, which affect both bulk and surface electronic states. While previous studies have focused on controlling symmetry via coupling to the crystal lattice, we demonstrate here an all-electronic mechanism based on photocurrent generation. Using second harmonic generation spectroscopy as a sensitive probe of symmetry changes, we observe an ultrafast breaking of time-reversal and spatial symmetries following femtosecond optical excitation in the prototypical type-I Weyl semimetal TaAs. Our results show that optically driven photocurrents can be tailored to explicitly break electronic symmetry in a generic fashion, opening up the possibility of driving phase transitions between symmetry-protected states on ultrafast timescales.
The authors demonstrate ultrafast symmetry breaking by optically driven photocurrents.
Journal Article
Polaronic Transport Induced by Competing Interfacial Magnetic Order in a La0.7Ca0.3MnO3/BiFeO3 Heterostructure
2014
Using ultrafast optical spectroscopy, we show that polaronic behavior associated with interfacial antiferromagnetic order is likely the origin of tunable magnetotransport upon switching the ferroelectric polarity in a La0.7Ca0.3MnO3/BiFeO3 (LCMO/BFO) heterostructure. This is revealed through the difference in dynamic spectral weight transfer between LCMO and LCMO/BFO at low temperatures, which indicates that transport in LCMO/BFO is polaronic in nature. This polaronic feature in LCMO/BFO decreases in relatively high magnetic fields due to the increased spin alignment, while no discernible change is found in the LCMO film at low temperatures. These results thus shed new light on the intrinsic mechanisms governing magnetoelectric coupling in this heterostructure, potentially offering a new route to enhancing multiferroic functionality.
Journal Article
Probing the Interplay between Quantum Charge Fluctuations and Magnetic Ordering in LuFe2O4
2013
The mechanisms producing strong coupling between electric and magnetic order in multiferroics are not always well understood, since their microscopic origins can be quite different. Hence, gaining a deeper understanding of magnetoelectric coupling in these materials is the key to their rational design. Here, we use ultrafast optical spectroscopy to show that the influence of magnetic ordering on quantum charge fluctuations via the double-exchange mechanism can govern the interplay between electric polarization and magnetism in the charge-ordered multiferroic LuFe
2
O
4
.
Journal Article
Coherent Spin-Phonon Coupling in the Layered Ferrimagnet Mn3Si2Te6
2023
We utilize ultrafast photoexcitation to drive coherent lattice oscillations in the layered ferrimagnetic crystal Mn3Si2Te6, which significantly stiffen below the magnetic ordering temperature. We suggest that this is due to an exchange-mediated contraction of the lattice, stemming from strong magneto-structural coupling in this material. Additionally, simulations of the transient incoherent dynamics reveal the importance of spin relaxation channels mediated by optical and acoustic phonon scattering. Our findings highlight the importance of spin-lattice coupling in van der Waals magnets and a promising route for their dynamic optical control through their intertwined electronic, lattice, and spin degrees of freedom.
Ultrafast Suppression of the Ferroelectric Instability in KTaO\\(_3\\)
by
Rondinelli, James M
,
Gu, Mingqiang
,
de la Peña, G
in
Brillouin zones
,
Charge density
,
Charge transfer
2022
We use an x-ray free-electron laser to study the ultrafast lattice dynamics following above band-gap photoexcitation of the incipient ferroelectric potassium-tantalate, \\kto. % We use ultrafast near-UV (central wavelength 266\\,nm and 50 fs pulse duration) laser light to photoexcite charge carriers across the gap and probe the ultrafast lattice dynamics by recording the x-ray diffuse intensity throughout multiple Brillouin zones using pulses from the Linac Coherent Light Source (LCLS) (central wavelength 1.3\\,\\AA\\, and \\(< 10\\)~fs pulse duration). We observe changes in the diffuse intensity that we conclude are associated with a hardening of the soft transverse optical and transverse acoustic phonon branches along \\(\\Gamma\\) to \\(X\\) and \\(\\Gamma\\) to \\(M\\). Using ground- and excited-state interatomic force constants from density functional theory (DFT) and assuming the phonon populations can be described by a time-dependent temperature, we fit the quasi-equilibrium thermal diffuse intensity to the experimental time-dependent intensity. We obtain the instantaneous lattice temperature and density of photoexcited charge carriers as a function of time delay. The DFT calculations demonstrate that photoexcitation transfers charge from oxygen \\(2p\\) derived \\(\\pi\\)-bonding orbitals to Ta \\(5d\\) derived antibonding orbitals, further suppressing the ferroelectric instability and increasing the stability of the cubic, paraelectric structure.