Revealing the effect of interstitial oxygen on the low-energy crystal electric field excitations of ${\mathrm{Pr}}^{3+}$ in $\mathit{214}$-nickelates

Revealing the effect of interstitial oxygen on the low-energy crystal electric field excitations of $\Pr^{3 +}$ in $214$ -nickelates

Rajesh Dutta, Avishek Maity, Anna Marsicano, J. Ross Stewart, Matthias Opel, and Werner Paulus

Phys. Rev. B 105, 195147 – Published 27 May 2022

Abstract

We report an inelastic neutron scattering study (INS) on the low-energy crystal electric field (CEF) excitations of $\Pr_{2 - x} {Sr}_{x} {NiO}_{4 + δ}$ single crystals at various temperatures. The observed low- $E$ CEF level of the O-doped sample $(x = 0, δ \approx 0.24)$ at $\sim 5.5 meV$ appears at significantly lower energy than that of the Sr-doped sample $(x = 0.5, δ = 0.0)$ at $\sim 8.5 meV$ . Applying the point charge (PC) model calculation, this has been interpreted as an effect of the interstitial oxygen via lowering the local symmetry and modifying the CEF environment of the central rare earth $\Pr^{3 +}$ $({}^{3}H_{4})$ ions.

Received 2 February 2022
Revised 5 April 2022
Accepted 18 May 2022

DOI:https://doi.org/10.1103/PhysRevB.105.195147

Physics Subject Headings (PhySH)

Electronic structure Magnetism

Antiferromagnets Strongly correlated systems

Crystal-field theory Inelastic neutron scattering

Condensed Matter, Materials & Applied Physics

Authors & Affiliations

Rajesh Dutta ^1,2,*, Avishek Maity ^3,†, Anna Marsicano ⁴, J. Ross Stewart⁵, Matthias Opel ⁶, and Werner Paulus ⁴

¹Institut für Kristallographie, RWTH Aachen Universität, 52066 Aachen, Germany
²Jülich Centre for Neutron Science at Heinz Maier-Leibnitz Zentrum, 85747 Garching, Germany
³Heinz Maier-Leibnitz Zentrum, Technische Universität München, 85747 Garching, Germany
⁴Institut Charles Gerhardt Montpellier, Université de Montpellier, 34095 Montpellier, France
⁵ISIS Neutron and Muon Source, Rutherford Appleton Laboratory, Didcot OX11 0QX, United Kingdom
⁶Walther-Meißner-Institut, Bayerische Akademie der Wissenschaften, 85748 Garching, Germany

^*Corresponding author: rajesh.dutta@frm2.tum.de
^†Corresponding author: avishek.maity@frm2.tum.de

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Vol. 105, Iss. 19 — 15 May 2022

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Figure 1
(Left) Capped-square antiprism CEF environment of $\Pr^{3 +}$ ion with fourfold or twofold rotational $z$ axis (black arrow) of the local point symmetry in case of $4 / m m m$ or $m m m$ , respectively. (Right) CEF environment with an extra $O_{int}$ (green).
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Figure 2
The INS spectra of PSNO measured at MAPS spectrometer with incident neutron energy $E_{i}$ = 60 meV at (a) 10 and (b) 150 K. Corresponding 1D line cuts at (100) with 0.95 $\leq Δ h \leq$ 1.05 (r.l.u) are shown in (c) and (d) with vertical error bars, where the solid green lines represent the calculated CEF excitations from the PC model. Inverse magnetic susceptibility along the crystallographic (e) $a$ and (f) $c$ axes where the solid red lines are the calculated inverse susceptibility of $\Pr^{3 +}$ using PC model.
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Figure 3
(a) The INS spectra of PNO measured at MAPS spectrometer with incident neutron energy $E_{i}$ = 60 meV at 5 K and the corresponding 1D line cuts at (100) with $0.95 \leq Δ h \leq$ 1.05 (r.l.u) are shown in (b) with vertical error bars, where the solid lines represent the calculated CEF excitations from the point charge (PC) model with two sets of CEF environment. Inverse magnetic susceptibility along the crystallographic (c) $a$ and (d) $c$ axes where the solid lines are the calculated susceptibility using PC models.
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Figure 4
(a) Integrated intensity of the INS spectrum of PSNO over the energy range 6 $\leq Δ E \leq$ 10 meV in Fig. 2 where the orange solid line represents the calculated magnetic form factor of $\Pr^{3 +}$ ion. (b) Integrated intensity of the INS spectrum of PSNO around the elastic scattering line over the energy range $- 2 \leq Δ E \leq 2 meV$ where the flat green solid line is the eye guide to zero intensity. In both cases the intensity integration has been performed taking into account fixed $- 0.3 \leq Δ k \leq - 0.2$ along ( $h, - 0.1, 0$ ). Strong intense peaks in (b) are coming from Bragg scattering. (c) Integrated intensity of the INS spectrum of PNO over the energy range $- 2 \leq Δ E \leq 2 meV$ (red), 4 $\leq Δ E \leq$ 8 meV (cyan) and $- 12 \leq Δ E \leq 8 meV$ (blue), where the grey solid line represents the calculated magnetic form factor of $\Pr^{3 +}$ ion. The intensity integration has been performed taking into account fixed $- 0.3 \leq Δ k \leq - 0.2$ along ( $h, - 0.1, 0$ ).
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Figure 5
Measured and simulated magnetization curves along the crystallographic $a$ and $c$ axes for the sample [(a) and (b)] PSNO and [(c) and (d)] PNO.
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Figure 6
3D plots of saturation magnetization representing the Pr single ion anisotropies of PSNO and PNO, in various directions at 10 K computed from the CEF parameters using the field of 150 T. The colored traces indicate the outline of the 3D figure along the $x, y$ , and $z$ directions.
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Physical Review B

covering condensed matter and materials physics

Revealing the effect of interstitial oxygen on the low-energy crystal electric field excitations of $\Pr^{3 +}$ in $214$ -nickelates

Rajesh Dutta, Avishek Maity, Anna Marsicano, J. Ross Stewart, Matthias Opel, and Werner Paulus

Phys. Rev. B 105, 195147 – Published 27 May 2022

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Revealing the effect of interstitial oxygen on the low-energy crystal electric field excitations of Pr3+ in 214-nickelates

Rajesh Dutta, Avishek Maity, Anna Marsicano, J. Ross Stewart, Matthias Opel, and Werner Paulus

Phys. Rev. B 105, 195147 – Published 27 May 2022

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Revealing the effect of interstitial oxygen on the low-energy crystal electric field excitations of $\Pr^{3 +}$ in $214$ -nickelates