Ligand-field helical luminescence in a 2D ferromagnetic insulator

Seyler, Kyle L.; Zhong, Ding; Klein, Dahlia R.; Gao, Shiyuan; Zhang, Xiaoou; Huang, Bevin; Navarro-Moratalla, Efren; Yang, Li; Cobden, David H.; McGuire, Michael A.; Yao, Wang; Xiao, Di; Jarillo-Herrero, Pablo; Xu, Xiaodong

doi:10.1038/s41567-017-0006-7

Title: Ligand-field helical luminescence in a 2D ferromagnetic insulator

Abstract

Bulk chromium tri-iodide (CrI₃) has long been known as a layered van der Waals ferromagnet. However, its monolayer form was only recently isolated and confirmed to be a truly two-dimensional (2D) ferromagnet, providing a new platform for investigating light–matter interactions and magneto-optical phenomena in the atomically thin limit. Here in this paper, we report spontaneous circularly polarized photoluminescence in monolayer CrI₃ under linearly polarized excitation, with helicity determined by the monolayer magnetization direction. In contrast, the bilayer CrI₃ photoluminescence exhibits vanishing circular polarization, supporting the recently uncovered anomalous antiferromagnetic interlayer coupling in CrI₃ bilayers. Distinct from the Wannier–Mott excitons that dominate the optical response in well-known 2D van der Waals semiconductors, our absorption and layer-dependent photoluminescence measurements reveal the importance of ligand-field and charge-transfer transitions to the optoelectronic response of atomically thin CrI₃. We attribute the photoluminescence to a parity-forbidden d–d transition characteristic of Cr³⁺ complexes, which displays broad linewidth due to strong vibronic coupling and thickness-independent peak energy due to its localized molecular orbital nature.

Authors:

Seyler, Kyle L. ^[1]; Zhong, Ding ^[1]; Klein, Dahlia R. ^[2]; Gao, Shiyuan ^[3]; Zhang, Xiaoou ^[4]; Huang, Bevin ^[1]; Navarro-Moratalla, Efren ^[2]; Yang, Li ^[3];

^[1];

^[5];

^[6]; Xiao, Di ^[4]; Jarillo-Herrero, Pablo ^[2];

^[7]

Univ. of Washington, Seattle, WA (United States). Dept. of Physics
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Physics
Washington Univ., St. Louis, MO (United States). Dept. of Physics
Carnegie Mellon Univ., Pittsburgh, PA (United States). Dept. of Physics
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Univ. of Hong Kong (China). Dept. of Physics and Center of Theoretical and Computational Physics
Univ. of Washington, Seattle, WA (United States). Dept. of Physics, and Dept. of Materials Science and Engineering

Publication Date:: 2017-12-04

Research Org.:: Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1430601

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Nature Physics

Additional Journal Information:: Journal Volume: 14; Journal Issue: 3; Journal ID: ISSN 1745-2473

Publisher:: Nature Publishing Group (NPG)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Seyler, Kyle L., Zhong, Ding, Klein, Dahlia R., Gao, Shiyuan, Zhang, Xiaoou, Huang, Bevin, Navarro-Moratalla, Efren, Yang, Li, Cobden, David H., McGuire, Michael A., Yao, Wang, Xiao, Di, Jarillo-Herrero, Pablo, and Xu, Xiaodong. Ligand-field helical luminescence in a 2D ferromagnetic insulator.  United States: N. p., 2017. 
Web.  doi:10.1038/s41567-017-0006-7.

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                    Seyler, Kyle L., Zhong, Ding, Klein, Dahlia R., Gao, Shiyuan, Zhang, Xiaoou, Huang, Bevin, Navarro-Moratalla, Efren, Yang, Li, Cobden, David H., McGuire, Michael A., Yao, Wang, Xiao, Di, Jarillo-Herrero, Pablo, & Xu, Xiaodong. Ligand-field helical luminescence in a 2D ferromagnetic insulator.  United States.  https://doi.org/10.1038/s41567-017-0006-7

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                    Seyler, Kyle L., Zhong, Ding, Klein, Dahlia R., Gao, Shiyuan, Zhang, Xiaoou, Huang, Bevin, Navarro-Moratalla, Efren, Yang, Li, Cobden, David H., McGuire, Michael A., Yao, Wang, Xiao, Di, Jarillo-Herrero, Pablo, and Xu, Xiaodong. Mon .  
"Ligand-field helical luminescence in a 2D ferromagnetic insulator".  United States.  https://doi.org/10.1038/s41567-017-0006-7.  https://www.osti.gov/servlets/purl/1430601.

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@article{osti_1430601,

  title        = {Ligand-field helical luminescence in a 2D ferromagnetic insulator},

  author       = {Seyler, Kyle L. and Zhong, Ding and Klein, Dahlia R. and Gao, Shiyuan and Zhang, Xiaoou and Huang, Bevin and Navarro-Moratalla, Efren and Yang, Li and Cobden, David H. and McGuire, Michael A. and Yao, Wang and Xiao, Di and Jarillo-Herrero, Pablo and Xu, Xiaodong},

  abstractNote = {Bulk chromium tri-iodide (CrI3) has long been known as a layered van der Waals ferromagnet. However, its monolayer form was only recently isolated and confirmed to be a truly two-dimensional (2D) ferromagnet, providing a new platform for investigating light–matter interactions and magneto-optical phenomena in the atomically thin limit. Here in this paper, we report spontaneous circularly polarized photoluminescence in monolayer CrI3 under linearly polarized excitation, with helicity determined by the monolayer magnetization direction. In contrast, the bilayer CrI3 photoluminescence exhibits vanishing circular polarization, supporting the recently uncovered anomalous antiferromagnetic interlayer coupling in CrI3 bilayers. Distinct from the Wannier–Mott excitons that dominate the optical response in well-known 2D van der Waals semiconductors, our absorption and layer-dependent photoluminescence measurements reveal the importance of ligand-field and charge-transfer transitions to the optoelectronic response of atomically thin CrI3. We attribute the photoluminescence to a parity-forbidden d–d transition characteristic of Cr3+ complexes, which displays broad linewidth due to strong vibronic coupling and thickness-independent peak energy due to its localized molecular orbital nature.},

  doi          = {10.1038/s41567-017-0006-7},

  journal      = {Nature Physics},

  number       = 3,

  volume       = 14,

  place        = {United States},

  year         = {2017},

  month        = {12}

}

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Controlling magnetism via electric fields addresses fundamental questions of magnetic phenomena and phase transitions, and enables the development of electrically coupled spintronic devices, such as voltage-controlled magnetic memories with low operation energy. Previous studies on dilute magnetic semiconductors such as (Ga,Mn)As and (In,Mn)Sb have demonstrated large modulations of the Curie temperatures and coercive fields by altering the magnetic anisotropy and exchange interaction. Owing to their unique magnetic properties, the recently reported two-dimensional magnets provide a new system for studying these features. For instance, a bilayer of chromium triiodide (CrI₃) behaves as a layered antiferromagnet with a magnetic field-driven metamagnetic transition.more »« less
Cited by 636
https://doi.org/10.1038/s41565-018-0121-3

Full Text Available
Valley Manipulation by Optically Tuning the Magnetic Proximity Effect in WSe₂/CrI₃ Heterostructures

Journal Article Seyler, Kyle L. ; Zhong, Ding ; Huang, Bevin ; ... - Nano Letters

Monolayer valley semiconductors, such as tungsten diselenide (WSe₂), possess valley pseudospin degrees of freedom that are optically addressable but degenerate in energy. Lifting the energy degeneracy by breaking time-reversal symmetry is vital for valley manipulation. This has been realized by directly applying magnetic fields or via pseudomagnetic fields generated by intense circularly polarized optical pulses. However, sweeping large magnetic fields is impractical for devices, and the pseudomagnetic fields are only effective in the presence of ultrafast laser pulses. The recent rise of two-dimensional (2D) magnets unlocks new approaches to controlling valley physics via van der Waals heterostructure engineering. Here, wemore »« less
Cited by 203
https://doi.org/10.1021/acs.nanolett.8b01105

Full Text Available

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Title: Ligand-field helical luminescence in a 2D ferromagnetic insulator

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Citation Formats

Magnetization, Resonance, and Optical Properties of the Ferromagnet CrI 3 journal, March 1965

Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged and free excitons journal, September 2013

Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals journal, April 2017

Effect of magnetic ordering on the optical properties of transition-metal halides: Ni Cl 2 , Ni Br 2 , Cr Cl 3 , and Cr Br 3 journal, March 1984

Insulating Ferromagnetic Spinels journal, September 1965

Spin and pseudospins in layered transition metal dichalcogenides journal, April 2014

Magnetotransport properties of p -type (In,Mn)As diluted magnetic III-V semiconductors journal, April 1992

Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides journal, March 2016

Coupling of Crystal Structure and Magnetism in the Layered, Ferromagnetic Insulator CrI 3 journal, January 2015

Dielectric Spectroscopy of Ferromagnetic Semiconductors journal, July 1957

Refraction and Dispersion of Synthetic Sapphire journal, January 1962

The optical electrical and magnetic properties of the europium chalcogenides and the rare earth pnictides journal, July 1972

Ising-Type Magnetic Ordering in Atomically Thin FePS 3 journal, November 2016

Spectroscopic studies of the two-dimensional magnetic insulators chromium trichloride and chromium tribromide—I journal, January 1979

Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit journal, June 2017

On the Magnetic Properties of a CrBr 3 Single Crystal journal, September 1960

Intrinsic Optical Properties of CrCl3 journal, January 1970

Valleytronics in 2D materials journal, August 2016

Diluted magnetic semiconductors journal, August 1988

Optical properties of III-Mn-V ferromagnetic semiconductors journal, December 2008

(Ga,Mn)As: A new diluted magnetic semiconductor based on GaAs journal, July 1996

Magneto-optical properties of ferromagnetic chromium trihalides journal, September 1966

Dilute ferromagnetic semiconductors: Physics and spintronic structures journal, March 2014

Charge-transfer transitions in chromium trihalides journal, October 1996

Magneto-optical properties of ferromagnetic chromium trihalides journal, April 1966

Insulating Ferromagnetic Spinels journal, September 1965

Discovery of Intrinsic Ferromagnetism in Two-Dimensional van der Waals Crystals conference, January 2017

Spectroscopic studies of the two-dimensional magnetic insulators chromium trichloride and chromium tribromide—II journal, January 1979

Optical Properties of III-Mn-V Ferromagnetic Semiconductors text, January 2008

Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit text, January 2017

New Frontiers on van der Waals Layered Metal Phosphorous Trichalcogenides journal, July 2018

Lattice Dynamics, Phonon Chirality, and Spin–Phonon Coupling in 2D Itinerant Ferromagnet Fe 3 GeTe 2 journal, September 2019

Controlling Magnetic and Optical Properties of the van der Waals Crystal CrCl 3− x Br x via Mixed Halide Chemistry journal, May 2018

Ultrathin Magnetic 2D Single‐Crystal CrSe journal, March 2019

Intrinsic Van Der Waals Magnetic Materials from Bulk to the 2D Limit: New Frontiers of Spintronics journal, May 2019

Raman fingerprint of two terahertz spin wave branches in a two-dimensional honeycomb Ising ferromagnet journal, November 2018

Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators journal, May 2019

Switchable magnetic bulk photovoltaic effect in the two-dimensional magnet CrI3 journal, August 2019

Two-dimensional itinerant ferromagnetism in atomically thin Fe3GeTe2 journal, August 2018

Electrical control of 2D magnetism in bilayer CrI3 journal, April 2018

Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3 journal, January 2020

Routing the emission of a near-surface light source by a magnetic field journal, August 2018

Enhancement of interlayer exchange in an ultrathin two-dimensional magnet journal, September 2019

Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3 journal, July 2019

Anisotropic magnetocaloric effect in Fe3−xGeTe2 journal, September 2019

Micromagnetometry of two-dimensional ferromagnets journal, September 2019

Probing and controlling magnetic states in 2D layered magnetic materials journal, September 2019

Distinct spin–lattice and spin–phonon interactions in monolayer magnetic CrI 3 journal, January 2018

Prediction of intrinsic two dimensional ferromagnetism realized quantum anomalous Hall effect journal, January 2019

Ferromagnetism in magnesium chloride monolayer with an unusually large spin-up gap journal, January 2018

Ferromagnetism in a semiconducting Janus NbSe hydride monolayer journal, January 2018

Two-dimensional transition-metal halide CoBr 3 with spin-polarized Dirac cone journal, January 2019

Lanthanide f 7 metalloxenes – a class of intrinsic 2D ferromagnets journal, January 2019

2D ferromagnetism in europium/graphene bilayers journal, January 2020

Biaxial strain induced band transition and valley–spin coupling in the ferromagnetic semiconducting WSe 2 /1T-FeCl 2 heterostructure journal, January 2019

Strain controlling transport properties of heterostructure composed of monolayer CrI 3 journal, May 2019

Ultrasensitive negative photoresponse in 2D Cr 2 Ge 2 Te 6 photodetector with light-induced carrier trapping journal, September 2018

Half-metallicity in two-dimensional Co 2 Se 3 monolayer with superior mechanical flexibility journal, September 2018

Calculating critical temperatures for ferromagnetic order in two-dimensional materials journal, December 2018

Growth and stabilization of two-dimensional multiferroics MnI 2 journal, May 2019

Recent progress of spintronics based on emerging 2D materials: CrI 3 and Xenes journal, December 2019

Strain-Induced Room-Temperature Ferromagnetic Semiconductors with Large Anomalous Hall Conductivity in Two-Dimensional Cr 2 Ge 2 Se 6 journal, July 2019

CoB 6 monolayer: A robust two-dimensional ferromagnet journal, January 2019

2D ferromagnetism in layered inorganic-organic hybrid perovskites journal, December 2019

Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling journal, May 2018

Probing magnetism in 2D materials at the nanoscale with single-spin microscopy journal, April 2019

Routing the emission of a near-surface light source by a magnetic field preprint, January 2017

Electrical Control of 2D Magnetism in Bilayer CrI3 text, January 2018

Two-Dimensional Itinerant Ising Ferromagnetism in Atomically thin Fe3GeTe2 text, January 2018

Calculating critical temperatures for ferromagnetic order in two-dimensional materials text, January 2018

Probing magnetism in 2D materials at the nanoscale with single spin microscopy text, January 2019

Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators text, January 2019

Anisotropic magnetocaloric effect in Fe$_{3-x}$GeTe$_2$ text, January 2019

Magnetization, Resonance, and Optical Properties of the Ferromagnet CrI ₃
journal, March 1965

Defects activated photoluminescence in two-dimensional semiconductors: interplay between bound, charged and free excitons
journal, September 2013

Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals
journal, April 2017

Effect of magnetic ordering on the optical properties of transition-metal halides: Ni ${Cl}_{2}$ , Ni ${Br}_{2}$ , Cr ${Cl}_{3}$ , and Cr ${Br}_{3}$
journal, March 1984

Insulating Ferromagnetic Spinels
journal, September 1965

Spin and pseudospins in layered transition metal dichalcogenides
journal, April 2014

Magnetotransport properties of p -type (In,Mn)As diluted magnetic III-V semiconductors
journal, April 1992

Photonics and optoelectronics of 2D semiconductor transition metal dichalcogenides
journal, March 2016

Coupling of Crystal Structure and Magnetism in the Layered, Ferromagnetic Insulator CrI ₃
journal, January 2015

Dielectric Spectroscopy of Ferromagnetic Semiconductors
journal, July 1957

Refraction and Dispersion of Synthetic Sapphire
journal, January 1962

The optical electrical and magnetic properties of the europium chalcogenides and the rare earth pnictides
journal, July 1972

Ising-Type Magnetic Ordering in Atomically Thin FePS ₃
journal, November 2016

Spectroscopic studies of the two-dimensional magnetic insulators chromium trichloride and chromium tribromide—I
journal, January 1979

Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit
journal, June 2017

On the Magnetic Properties of a CrBr ₃ Single Crystal
journal, September 1960

Intrinsic Optical Properties of CrCl3
journal, January 1970

Valleytronics in 2D materials
journal, August 2016

Diluted magnetic semiconductors
journal, August 1988

Optical properties of III-Mn-V ferromagnetic semiconductors
journal, December 2008

(Ga,Mn)As: A new diluted magnetic semiconductor based on GaAs
journal, July 1996

Magneto-optical properties of ferromagnetic chromium trihalides
journal, September 1966

Dilute ferromagnetic semiconductors: Physics and spintronic structures
journal, March 2014

Charge-transfer transitions in chromium trihalides
journal, October 1996

Magneto-optical properties of ferromagnetic chromium trihalides
journal, April 1966

Insulating Ferromagnetic Spinels
journal, September 1965

Discovery of Intrinsic Ferromagnetism in Two-Dimensional van der Waals Crystals
conference, January 2017

Spectroscopic studies of the two-dimensional magnetic insulators chromium trichloride and chromium tribromide—II
journal, January 1979

Optical Properties of III-Mn-V Ferromagnetic Semiconductors
text, January 2008

Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
text, January 2017

New Frontiers on van der Waals Layered Metal Phosphorous Trichalcogenides
journal, July 2018

Lattice Dynamics, Phonon Chirality, and Spin–Phonon Coupling in 2D Itinerant Ferromagnet Fe ₃ GeTe ₂
journal, September 2019

Controlling Magnetic and Optical Properties of the van der Waals Crystal CrCl ₃₋ _x Br _x via Mixed Halide Chemistry
journal, May 2018

Ultrathin Magnetic 2D Single‐Crystal CrSe
journal, March 2019

Intrinsic Van Der Waals Magnetic Materials from Bulk to the 2D Limit: New Frontiers of Spintronics
journal, May 2019

Raman fingerprint of two terahertz spin wave branches in a two-dimensional honeycomb Ising ferromagnet
journal, November 2018

Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
journal, May 2019

Switchable magnetic bulk photovoltaic effect in the two-dimensional magnet CrI3
journal, August 2019

Two-dimensional itinerant ferromagnetism in atomically thin Fe3GeTe2
journal, August 2018

Electrical control of 2D magnetism in bilayer CrI3
journal, April 2018

Tuning inelastic light scattering via symmetry control in the two-dimensional magnet CrI3
journal, January 2020

Routing the emission of a near-surface light source by a magnetic field
journal, August 2018

Enhancement of interlayer exchange in an ultrathin two-dimensional magnet
journal, September 2019

Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI3
journal, July 2019

Anisotropic magnetocaloric effect in Fe3−xGeTe2
journal, September 2019

Micromagnetometry of two-dimensional ferromagnets
journal, September 2019

Probing and controlling magnetic states in 2D layered magnetic materials
journal, September 2019

Distinct spin–lattice and spin–phonon interactions in monolayer magnetic CrI ₃
journal, January 2018

Prediction of intrinsic two dimensional ferromagnetism realized quantum anomalous Hall effect
journal, January 2019

Ferromagnetism in magnesium chloride monolayer with an unusually large spin-up gap
journal, January 2018

Ferromagnetism in a semiconducting Janus NbSe hydride monolayer
journal, January 2018

Two-dimensional transition-metal halide CoBr ₃ with spin-polarized Dirac cone
journal, January 2019

Lanthanide f ⁷ metalloxenes – a class of intrinsic 2D ferromagnets
journal, January 2019

2D ferromagnetism in europium/graphene bilayers
journal, January 2020

Biaxial strain induced band transition and valley–spin coupling in the ferromagnetic semiconducting WSe ₂ /1T-FeCl ₂ heterostructure
journal, January 2019

Strain controlling transport properties of heterostructure composed of monolayer CrI ₃
journal, May 2019

Ultrasensitive negative photoresponse in 2D Cr ₂ Ge ₂ Te ₆ photodetector with light-induced carrier trapping
journal, September 2018

Half-metallicity in two-dimensional Co ₂ Se ₃ monolayer with superior mechanical flexibility
journal, September 2018

Calculating critical temperatures for ferromagnetic order in two-dimensional materials
journal, December 2018

Growth and stabilization of two-dimensional multiferroics MnI ₂
journal, May 2019

Recent progress of spintronics based on emerging 2D materials: CrI ₃ and Xenes
journal, December 2019

Strain-Induced Room-Temperature Ferromagnetic Semiconductors with Large Anomalous Hall Conductivity in Two-Dimensional ${Cr}_{2} {Ge}_{2} {Se}_{6}$
journal, July 2019

${CoB}_{6}$ monolayer: A robust two-dimensional ferromagnet
journal, January 2019

2D ferromagnetism in layered inorganic-organic hybrid perovskites
journal, December 2019

Probing magnetism in 2D van der Waals crystalline insulators via electron tunneling
journal, May 2018

Probing magnetism in 2D materials at the nanoscale with single-spin microscopy
journal, April 2019

Routing the emission of a near-surface light source by a magnetic field
preprint, January 2017

Electrical Control of 2D Magnetism in Bilayer CrI3
text, January 2018

Two-Dimensional Itinerant Ising Ferromagnetism in Atomically thin Fe3GeTe2
text, January 2018

Calculating critical temperatures for ferromagnetic order in two-dimensional materials
text, January 2018

Probing magnetism in 2D materials at the nanoscale with single spin microscopy
text, January 2019

Physical origin of giant excitonic and magneto-optical responses in two-dimensional ferromagnetic insulators
text, January 2019

Anisotropic magnetocaloric effect in Fe$_{3-x}$GeTe$_2$
text, January 2019