Decoupling spin-orbital correlations in a layered manganite amidst ultrafast hybridized charge-transfer band excitation

L. Shen; S. A. Mack; G. Dakovski; G. Coslovich; O. Krupin; M. Hoffmann; S. W. Huang; Y. D. Chuang; J. A. Johnson; S. Lieu; S. Zohar; C. Ford; M. Kozina; W. Schlotter; M. P. Minitti; J. Fujioka; R. Moore; W. S. Lee; Z. Hussain; Y. Tokura; P. Littlewood; J. J. Turner

doi:10.1103/PhysRevB.101.201103

Decoupling spin-orbital correlations in a layered manganite amidst ultrafast hybridized charge-transfer band excitation

L. Shen, S. A. Mack, G. Dakovski, G. Coslovich, O. Krupin, M. Hoffmann, S. W. Huang, Y. D. Chuang, J. A. Johnson, S. Lieu, S. Zohar, C. Ford, M. Kozina, W. Schlotter, M. P. Minitti, J. Fujioka, R. Moore, W. S. Lee, Z. Hussain, Y. TokuraP. Littlewood, J. J. Turner

Quantum Heterostructures

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4 Scopus citations

Abstract

In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced d1d0→d0d1 excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods-both femtosecond resonant X-ray diffraction and optical reflectivity-to demonstrate that the orbital response in the layered manganite Nd_1-xSr_1+xMnO₄(x=2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical d1d0→d0d1 transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the d0→d1L, where L denotes a hole in the oxygen band. This finding may pave a different avenue for selectively manipulating specific types of order in complex materials of this class.

Original language	English
Article number	201103
Journal	Physical Review B
Volume	101
Issue number	20
DOIs	https://doi.org/10.1103/PhysRevB.101.201103
State	Published - May 15 2020

Funding

We acknowledge useful discussions with R. Schoenlein, A. Sakdinawat, S. Johnson, and U. Staub. Special thanks to D. Green, K. Thompson, and S. Curry. We are grateful for data support from J. Thayer and C. O'Grady. This work was supported by the U. S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-76SF00515. The use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, was also supported under the same contract. Y-D.C. acknowledges the support from the Advanced Light Source, a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231. J.J.T. acknowledges support from the U.S. DOE, Office of Science, Basic Energy Sciences through the Early Career Research Program. This work was supported by the U. S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division, under Contract No. DE-AC02-76SF00515. The use of the Linac Coherent Light Source (LCLS), SLAC National Accelerator Laboratory, was also supported under the same contract. Y-D.C. acknowledges the support from the Advanced Light Source, a DOE Office of Science User Facility under Contract No. DE-AC02-05CH11231. J.J.T. acknowledges support from the U.S. DOE, Office of Science, Basic Energy Sciences through the Early Career Research Program.

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Shen, L., Mack, S. A., Dakovski, G., Coslovich, G., Krupin, O., Hoffmann, M., Huang, S. W., Chuang, Y. D., Johnson, J. A., Lieu, S., Zohar, S., Ford, C., Kozina, M., Schlotter, W., Minitti, M. P., Fujioka, J., Moore, R., Lee, W. S., Hussain, Z., ... Turner, J. J. (2020). Decoupling spin-orbital correlations in a layered manganite amidst ultrafast hybridized charge-transfer band excitation. Physical Review B, 101(20), Article 201103. https://doi.org/10.1103/PhysRevB.101.201103

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title = "Decoupling spin-orbital correlations in a layered manganite amidst ultrafast hybridized charge-transfer band excitation",

abstract = "In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced d1d0→d0d1 excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods-both femtosecond resonant X-ray diffraction and optical reflectivity-to demonstrate that the orbital response in the layered manganite Nd1-xSr1+xMnO4(x=2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical d1d0→d0d1 transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the d0→d1L, where L denotes a hole in the oxygen band. This finding may pave a different avenue for selectively manipulating specific types of order in complex materials of this class.",

author = "L. Shen and Mack, {S. A.} and G. Dakovski and G. Coslovich and O. Krupin and M. Hoffmann and Huang, {S. W.} and Chuang, {Y. D.} and Johnson, {J. A.} and S. Lieu and S. Zohar and C. Ford and M. Kozina and W. Schlotter and Minitti, {M. P.} and J. Fujioka and R. Moore and Lee, {W. S.} and Z. Hussain and Y. Tokura and P. Littlewood and Turner, {J. J.}",

note = "Publisher Copyright: {\textcopyright} 2020 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.",

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Shen, L, Mack, SA, Dakovski, G, Coslovich, G, Krupin, O, Hoffmann, M, Huang, SW, Chuang, YD, Johnson, JA, Lieu, S, Zohar, S, Ford, C, Kozina, M, Schlotter, W, Minitti, MP, Fujioka, J, Moore, R, Lee, WS, Hussain, Z, Tokura, Y, Littlewood, P & Turner, JJ 2020, 'Decoupling spin-orbital correlations in a layered manganite amidst ultrafast hybridized charge-transfer band excitation', Physical Review B, vol. 101, no. 20, 201103. https://doi.org/10.1103/PhysRevB.101.201103

TY - JOUR

T1 - Decoupling spin-orbital correlations in a layered manganite amidst ultrafast hybridized charge-transfer band excitation

AU - Shen, L.

AU - Mack, S. A.

AU - Dakovski, G.

AU - Coslovich, G.

AU - Krupin, O.

AU - Hoffmann, M.

AU - Huang, S. W.

AU - Chuang, Y. D.

AU - Johnson, J. A.

AU - Lieu, S.

AU - Zohar, S.

AU - Ford, C.

AU - Kozina, M.

AU - Schlotter, W.

AU - Minitti, M. P.

AU - Fujioka, J.

AU - Moore, R.

AU - Lee, W. S.

AU - Hussain, Z.

AU - Tokura, Y.

AU - Littlewood, P.

AU - Turner, J. J.

N1 - Publisher Copyright: © 2020 authors. Published by the American Physical Society. Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.

PY - 2020/5/15

Y1 - 2020/5/15

N2 - In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced d1d0→d0d1 excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods-both femtosecond resonant X-ray diffraction and optical reflectivity-to demonstrate that the orbital response in the layered manganite Nd1-xSr1+xMnO4(x=2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical d1d0→d0d1 transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the d0→d1L, where L denotes a hole in the oxygen band. This finding may pave a different avenue for selectively manipulating specific types of order in complex materials of this class.

AB - In the mixed-valence manganites, a near-infrared laser typically melts the orbital and spin order simultaneously, corresponding to the photoinduced d1d0→d0d1 excitations in the Mott-Hubbard bands of manganese. Here, we use ultrafast methods-both femtosecond resonant X-ray diffraction and optical reflectivity-to demonstrate that the orbital response in the layered manganite Nd1-xSr1+xMnO4(x=2/3) does not follow this scheme. At the photoexcitation saturation fluence, the orbital order is only diminished by a few percent in the transient state. Instead of the typical d1d0→d0d1 transition, a near-infrared pump in this compound promotes a fundamentally distinct mechanism of charge transfer, the d0→d1L, where L denotes a hole in the oxygen band. This finding may pave a different avenue for selectively manipulating specific types of order in complex materials of this class.

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U2 - 10.1103/PhysRevB.101.201103

DO - 10.1103/PhysRevB.101.201103

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SN - 2469-9950

VL - 101

JO - Physical Review B

JF - Physical Review B

IS - 20

M1 - 201103

ER -

Decoupling spin-orbital correlations in a layered manganite amidst ultrafast hybridized charge-transfer band excitation

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