Lattice Coherence Research Articles

High-Entropy Rock-Salt Surface Layer Stabilizes the Ultrahigh-Ni Single-Crystal Cathode.

Single-crystalline Ni-rich layered oxides are one of the most promising cathode materials for lithium-ion batteries due to their superior structural stability. However, sluggish lithium-ion diffusion kinetics and interfacial issues hinder their practical applications. These issues intensify with increasing Ni content in the ultrahigh-Ni regime (≥90%), significantly threatening the practical viability of the single-crystalline strategy for ultrahigh-Ni layered oxide cathodes. Herein, by developing a high-entropy coating strategy, we successfully constructed an epitaxial lattice-coherent high-entropy rock-salt layer (∼3 nm) via Zr and Al doping on the surface of the single-crystalline cathode LiNi0.92Co0.05Mn0.03O2 through an in situ modification process. The surface high-entropy rock-salt layer with tailored Ni valence and lattice coherence not only greatly improves lithium-ion diffusion kinetics but also suppresses interface parasitic reactions and surface structural degradations. The high-entropy surface layer-stabilized ultrahigh-Ni single-crystalline cathode (SC-Ni92-ZA) demonstrates significantly improved rate and cycling performances (127.5 mAh g-1 at 20C, capacity retention of 74.9% after 500 cycles at 1C) in a half-cell. The SC-Ni92-ZA exhibits a capacity retention of 87.1% after 600 cycles at 1C in a full-cell. This epitaxial lattice-coherent high-entropy coating strategy develops a promising avenue for developing high-capacity, long-life cathode materials.

Investigating the Impact of Stress on the Optical Properties of GaN-MX2 (M=Mo, W; X=S, Se) Heterojunctions Using the First Principles

This study used the first-principles-based CASTEP software to calculate the structural, electronic, and optical properties of heterojunctions based on single-layer GaN. GaN-MX2 exhibited minimal lattice mismatches, typically less than 3.5%, thereby ensuring lattice coherence. Notably, GaN-MoSe2 had the lowest binding energy, signifying its superior stability among the variants. When compared to single-layer GaN, which has an indirect band gap, all four heterojunctions displayed a smaller direct band gap. These heterojunctions were classified as type II. GaN-MoS2 and GaN-MoSe2 possessed relatively larger interface potential differences, hinting at stronger built-in electric fields. This resulted in an enhanced electron–hole separation ability. GaN-MoSe2 exhibited the highest value for the real part of the dielectric function. This suggests a superior electronic polarization capability under an electric field, leading to high electron mobility. GaN-MoSe2 possessed the strongest optical absorption capacity. Consequently, GaN-MoSe2 was inferred to possess the strongest photocatalytic capability. The band structure and optical properties of GaN-MoSe2 under applied pressure were further calculated. The findings revealed that stress significantly influenced the band gap width and light absorption capacity of GaN-MoSe2. Specifically, under a pressure of 5 GPa, GaN-MoSe2 demonstrated a significantly narrower band gap and enhanced absorption capacity compared to its intrinsic state. These results imply that the application of stress could potentially boost its photocatalytic performance, making it a promising candidate for various applications.

Evolution of surface conductivity in SmB6 under nonmagnetic (Yb2+) and magnetic (Eu2+) doping

Among of rare-earth (RE) hexaborides only two compounds SmB6 and YbB6 are discussed in literature to be members of a new class of 3D topological insulators. However, their ground states originate due to different physical mechanisms, including Kondo 4f-5d hybridization and 5d-2p band inversion, respectively. Here we report a comparative study of magnetotransport (resistivity and transverse magnetoresistance) measured on high quality single crystals of YbxSm1-xB6 and EuxSm1-xB6 solid solutions (x ≤ 0.05) at temperatures 1.7 − 300 K in magnetic fields up to 82 kOe. The choice of dopant was determined by the fact that the presence of magnetic/nonmagnetic (Eu2+/Yb2+) impurity in parent SmB6 matrix should lift/not lift the topological protection of surface states. Based on the two-gap paradigm the x-evolution of electron spectra in YbxSm1-xB6 and EuxSm1-xB6 was studied. Our data show that both the 4f lattice coherence (Eg) and the intrinsic gap (Ea) related to many-body states survive under RE doping at least for x ≈ 0.02 − 0.024. We also suggest that the point x(Eu) = 0.05 can be treated as an upper limit of the small gap closing in EuxSm1-xB6 materials. In YbxSm1-xB6 family a negative linear transverse magnetoresistance (TMR) was detected for the first time in the regime of surface conductivity (T < T∗ ≈ 5 K). The TMR anomaly at T∗ caused possibly by the topological protection of surface states in SmB6 is found to survive in Eu-doped compounds but disappears almost completely for Yb-doped compositions in the same fixed magnetic fields. This paradoxical observation is not consistent with general predictions of the topological Kondo insulator (TKI) model.

Building a robust surface structure toward stable ultrahigh-nickel cathodes

Ni-rich cathodes especially with Ni content over 90 % are promising next-generation cathode materials for advanced high energy lithium − ion batteries. However, in comparison with Ni ≤ 80 % Ni-rich cathodes, these ultrahigh Ni-rich materials face more severe challenges in terms of harmful H2 − H3 phase transformations and structural degradation during cycling. Herein, we present a robust surface structure composted of defect-rich disordered structures and LiF/Li2SiO3 coating for stabilizing the ultrahigh Ni-rich cathode LiNi0.96Co0.03Mn0.01O2 (NCM96) by modification with (NH4)2SiF6. The surface disordered structures including Li/TM mixing, spinel, and rock salt structure play a crucial role in inhibiting the irreversible H2-H3 phase transition and reducing lattice volume changes by lattice coherence effect. Moreover, the disordered surface in collaboration with the co-coating restrains the rapid growth of surface rock salt phase into the bulk, enhancing structural stability. The modified sample NSF-0.5 delivers a capacity of 238 mAh/g at 0.1C and maintains a capacity retention of 88.5 % at 0.5C after 100 cycles in half cell as well as 82.3 % at 1C after 300 cycles in full cell, significantly superior to the NCM96. The findings provide a simple and cost-effective surface modification strategy to enhance the structural stability and electrochemical performance of ultrahigh nickel cathodes for high-energy density LIBs.

Oscillation of interlayer coupling in epitaxial FePd|Ir|FePd(001) perpendicular synthetic antiferromagnet

L10 FePd is a promising candidate material for spin memory devices, especially when paired with Ir as an interlayer coupling layer, leading to significant interlayer exchange coupling (IEC) energy between ferromagnetic layers and strong perpendicular magnetic anisotropy. Synthetic antiferromagnets (SAFs) are emphasized for spintronic applications, offering advantages like quick magnetization switching and enhanced stability. This study presents findings on the influence of Ir spacer thickness on the structural and magnetic properties of FePd SAFs, highlighting lattice matching and coherence throughout the entire SAF structure and revealing a maximum interlayer exchange energy of 3 mJ/m2. We suggest the potential of this FePd|Ir|FePd system as a building block for future spintronic applications.

Nanoscale engineering of low-misfit TiB2/Al3(Sc,Zr)/α-Al multi-interface to improve strength-ductility synergy for direct energy deposited aluminum alloy

The nature of the interface between ceramic particle (CP) and metal matrix is critical to obtain solidification microstructures with optimal mechanical properties of CP-reinforced Al alloys in additive manufacturing. Generally, when the lattice misfit between the CP (e.g., TiB2) and the α-Al matrix is higher than 4%, the interfacial coherency reduces, lowering the effectiveness of CPs. Here, we demonstrate that an L12 three-dimensional compound (3DC), which possesses lattice misfit with α-Al lower than 1%, can be introduced in between TiB2 and α-Al via properly regulating the solidification cooling rate. In the 5TiB2/Al-4.5Mg-0.7Sc-0.2Zr (wt%) as a model system, the lattice coherence of the TiB2/α-Al interface is tailored by introducing a 10–30 nm thick Al3(Sc,Zr) 3DC interphase when the cooling rate is increased to ∼1000 °C/s. But, further increasing the cooling rate to ∼6800 °C/s, only Al3(Sc,Zr) two-dimensional compound (2DC) with an apparent lattice strain forms at the interface. Taking advantage of the cooling rate (102-103 oC/s) provided by laser direct energy deposition (L-DED), the low-misfit “TiB2/Al3(Sc,Zr) 3DC/α-Al” multi-structural interfaces are acquired, enabling the 3.56TiB2/Al-4.36Mg-0.72Sc-0.22Zr alloy as fabricated with L-DED to achieved improved strength-ductility synergy (yield strength 257 MPa, elongation 13.8%) due to the isotropically fine Al grain structure and the homogenous TiB2 particle dispersion. The outcome of this study provides fundamental knowledge on designing “ceramic/coherent primary interphase/metal matrix” multi-structural interfaces to improve the mechanical properties of engineering metallic materials manufactured by rapid solidification techniques, such as DED additive manufacturing (AM).

Evidence for ground state coherence in a two-dimensional Kondo lattice

Kondo lattices are ideal testbeds for the exploration of heavy-fermion quantum phases of matter. While our understanding of Kondo lattices has traditionally relied on complex bulk f-electron systems, transition metal dichalcogenide heterobilayers have recently emerged as simple, accessible and tunable 2D Kondo lattice platforms where, however, their ground state remains to be established. Here we present evidence of a coherent ground state in the 1T/1H-TaSe2 heterobilayer by means of scanning tunneling microscopy/spectroscopy at 340 mK. Our measurements reveal the existence of two symmetric electronic resonances around the Fermi energy, a hallmark of coherence in the spin lattice. Spectroscopic imaging locates both resonances at the central Ta atom of the charge density wave of the 1T phase, where the localized magnetic moment is held. Furthermore, the evolution of the electronic structure with the magnetic field reveals a non-linear increase of the energy separation between the electronic resonances. Aided by ab initio and auxiliary-fermion mean-field calculations, we demonstrate that this behavior is inconsistent with a fully screened Kondo lattice, and suggests a ground state with magnetic order mediated by conduction electrons. The manifestation of magnetic coherence in TMD-based 2D Kondo lattices enables the exploration of magnetic quantum criticality, Kondo breakdown transitions and unconventional superconductivity in the strict two-dimensional limit.

Interplay Between Strain and Thickness on the Effective Carrier Lifetime of Buffer-Mediated Epitaxial Germanium Probed by the Photoconductance Decay Technique

We report contactless effective minority carrier lifetime of epitaxially grown unstrained and in-plane <110> biaxially tensile-strained (001) germanium (ε-Ge) epilayers measured using microwave-reflectance photoconductance decay measurements. Strained Ge epilayers were grown using InxGa1–xAs linearly graded buffers on (001) GaAs substrates. Using homogeneous excitation of unstrained Ge epilayers, thickness-dependent separation of minority carrier lifetime components under low injection conditions yielded a bulk lifetime of 114 ± 2 ns and low surface recombination velocity of 21.3 ± 0.04 cm/s. More notably, an effective minority carrier lifetime of >100 ns obtained from sub-50 nm 1.6% tensile-strained Ge epilayers showed no degradation relative to the unstrained counterpart. Detailed material characterization using X-ray diffractometry revealed successful strain transfer of 0.61 and 0.89% to the Ge epilayers via InxGa1–xAs metamorphic buffers and confirms pseudomorphic growth. Lattice coherence observed at the ε-Ge epilayer and InxGa1–xAs buffer heterointerfaces via transmission electron microscopy substantiates the prime material quality achieved. The relatively high carrier lifetimes achieved are an indicator of excellent material quality and provide a path forward to realize low-threshold Ge laser sources.

Multiscale Phase-Contrast Tomography at BM18

Synchrotron phase-contrast micro-tomography is considered the gold standard in non-destructive volumetric imaging of millimeter and centimeter-sized objects. Micro-tomography beamlines are operating at many synchrotron radiation facilities, including the Extremely Brilliant Source (EBS) at the European Synchrotron Radiation Facility (ESRF). Applications favor objects which cannot be sufficiently resolved by state-of-the-art industrial micro-CT scanners. Synchrotron tomography features much superior time resolution, e.g., for in situ micro-CT, as well as superior photon flux, thus making this method suitable for Region of Interest scanning (i.e., multiresolution tomography). This report presents first results from the EBS' latest industrial beamline BM18, which was built for hierarchical propagation phase-contrast tomography. BM18 makes use of the exceptionally high coherence of the new ESRF-EBS lattice. Thanks to the wide polychromatic high-energy beam, one can scan and zoom into larger parts, e.g., from additive manufacturing or battery packs. In particular, BM18 allows for recording multiple scans at different resolutions ranging from 42 μm down to 0.6 μm, without the need to remove the object or manually change detectors. Free space propagation of up to 36 m yields excellent phase-contrast which in turn enhances the resolving power of the system. BM18 is generating an unprecedented amount of very large datasets. Consequently, novel strategies for data processing, storage and visualization are under development for this particular instrument.

Nitride-reinforced HfNbTaTiV high-entropy alloy with excellent room and elevated-temperature mechanical properties

Nitride-reinforced (HfNbTaTiV)90N10 high-entropy alloy aiming at high-temperature applications is designed in this paper. Abundant FCC nitride phases are formed in situ in theBCC matrix by arc melting technique, without complex deformation or heat treatment. The (HfNbTaTiV)90N10 alloy exhibits a remarkable yield strength of 2716 MPa and ultimate compressive strength of 2833 MPa with a plastic strain of 10% at room temperature. Besides, the alloy remains a high yield strength of 279 MPa at 1400 °C. The nitride phases play an essential role in maintaining the excellent strength-ductility combination at room temperature and enhancing the high-temperature softening resistance. Alternating BCC and FCC phases possess the semi-coherent interface, which not only strengthens the BCC matrix but also promotes the compatible deformation of the duplex microstructure. The lattice coherency structure of the semi-coherent interface is conducive to the slip transfer of partial dislocations through the interface, which facilitates the accommodation of plastic deformation. The cross-slip of the screw dislocations effectively eliminates stress concentration and leads to good ductility of the dual-phase alloy. The results demonstrate that the nitride phases achieve coordinate deformation with the matrix without deteriorating the ductility of the (HfNbTaTiV)90N10 alloy.

Lateral Heterostructures of Graphene and h-BN with Atomic Lattice Coherence and Tunable Rotational Order.

In-plane heterostructures of graphene and hexagonal boron nitride (h-BN)exhibit exceptional properties, which are highly sensitive to the structure of the alternating domains. Nevertheless, achieving accurate control over their structural properties, while keeping a high perfection at the graphene-h-BN boundaries, still remains a challenge. Here, the growth of lateral heterostructures of graphene and h-BN on Rh(110) surfaces is reported. The choice of the 2D material, grown firstly, determines the structural properties of the whole heterostructure layer, allowing to have control over the rotational order of the domains. The atomic-scale observation of the boundaries demonstrates a perfect lateral matching. In-plane heterostructures floating over an oxygen layer have been successfully obtained, enabling to observe intervalley scattering processes in graphene regions. The high tuning capabilities of these heterostructures, along with their good structural quality, even around the boundaries, suggest their usage as test beds for fundamental studies aiming at the development of novel nanomaterials with tailored properties.

Investigation of interfacial strength in nacre-mimicking tungsten heavy alloys for nuclear fusion applications

Tungsten heavy alloys have been proposed as plasma facing material components in nuclear fusion reactors and require experimental investigation in their confirmation. For this purpose, a 90W–7Ni–3Fe alloy has been selected and microstructurally manipulated to present a multiphase brick-and-mortar structure of W-phase ‘bricks’ surrounded by a ductile ‘mortar’. This work draws inspiration from nature to artificially imitate the extraordinary combination of strength and stiffness exhibited by mollusks and produce a nacre-mimicking metal matrix composite capable of withstanding the extremely hostile environment of the reactor interior and maintaining structural integrity. The underlying mechanisms behind this integrity have been probed through high-resolution structural and chemical characterization techniques and have revealed chemically diffuse phase boundaries exhibiting unexpected lattice coherency. These features have been attributed to an increase in the energy required for interfacial decohesion in these systems and the simultaneous expression of high strength and toughness in tungsten heavy alloys.

Ultrastrong spinodoid alloys enabled by electrochemical dealloying and refilling

We present an extreme case of composition-modulated nanomaterial formed by selective etching (dealloying) and electrochemical refilling. The product is a coarse-grain polycrystal consisting of two interwoven nanophases, with identical crystal structures and a cube-on-cube relationship, separated by smoothly curved semicoherent interfaces with high-density misfit dislocations. This material resembles spinodal alloys structurally, but its synthesis and composition modulation are spinodal-independent. Our Cu/Au "spinodoid" alloy demonstrates superior mechanical properties such as near-theoretical strength and single-phase-like behavior, owing to its fine composition modulation, large-scale coherence of crystal lattice, and smoothly shaped three-dimensional (3D) interface morphology. As a unique extension of spinodal alloy, the spinodoid alloy reported here reveals a number of possibilities to modulate the material's structure and composition down to the nanoscale, such that further improved properties unmatchable by conventional materials can be achieved.

Ultrafast Loss of Lattice Coherence in the Light-Induced Structural Phase Transition of V_{2}O_{3}.

In solids, the response of the lattice to photoexcitation is often described by the inertial evolution on an impulsively modified potential energy surface which leads to coherent motion. However, it remains unknown if vibrational coherence is sustained through a phase transition, during which coupling between modes can be strong and may lead to rapid loss of coherence. Here we use coherent phonon spectroscopy to track lattice coherence in the structural phase transition of V_{2}O_{3}. In both the low and high symmetry phases unique coherent phonon modes are generated at low fluence. However, coherence is lost when driving between the low and high symmetry phases. Our results suggest strongly damped noninertial dynamics dominate during the phase transition due to disorder and multimode coupling.

Innovative strategy to optimize the temperature-dependent lattice misfit and coherency of iridium-based γ/γ’ interfaces

Ir/Ir3X (X = Hf, Nb, Ta, Ti, V, and Zr) are promising dual-phase materials with high strength at ultrahigh temperatures. However, previous investigations revealed that the relatively large lattice misfit and small critical coherent diameters adversely impact the strength of the Ir/Ir3X interfaces. Herein, a novel strategy is proposed for modeling the ternary alloys by mixing two Ir3X binary alloys having both the negative and positive lattice misfit and to form fully coherent γ/γ’ interfaces with Ir. The ternary Ir3XmVn alloys exhibit good high-temperature performance, such as high bulk modulus (∼200–240 GPa) at 2000 K. Remarkably, the lattice misfit of Ir3XmVn alloys with the Ir matrix (−0.8 %–0%) shows a significant reduction compared to that of the binary Ir3X alloys (−0.6 %–+2.4 %) in the 0–2000 K temperature range. The reduction in lattice misfit is accompanied by an increase in the critical coherent diameters.

Band structures in orientation-controlled CuI thin films under epitaxial strain

Cuprous iodide (CuI) is a wide bandgap (\ensuremath{\sim}3.1 eV) semiconductor of great recent interest because of its high transparency, high hole conductivity, large exciton binding energy, and sizable spin-orbit interaction. However, studies on single-crystalline thin films have been scarcely reported. Here, we report on the epitaxial growth of single-crystalline CuI films and their optical characterization to elucidate the modification of band structure caused by the anisotropic strain. Thin films were grown by molecular beam epitaxy on nearly lattice-matched (only 0.1%-mismatched) InAs substrates with (001), (110), and (111) crystal orientation, yielding pseudomorphic structures with high lattice coherence and atomic-level flatness. Both reflectance and photoluminescence spectra exhibit sharp exciton profiles over a wide temperature range. We assign the exciton transition energies to deduce the band structure modifications associated with the epitaxial strain varying with temperature and growth orientation. Furthermore, we determine the deformation potentials which relate the strain to the band structure modification. The systematic studies of the strain effect for CuI thin films on various substrate planes will pave the way for the future optoelectronic application of CuI-based heterostructures.

Low-pressure acidic ammonothermal growth of 2-inch-diameter nearly bowing-free bulk GaN crystals

Seeded growth of 2-inch-diameter GaN crystals via low-pressure (∼100 MPa) acidic ammonothermal method is demonstrated. Nearly bowing- and mosaic-free GaN crystals exhibiting full-width at half-maximum values for the 0002 X-ray rocking curves below 20 arcsec were achieved on high lattice coherency c-plane SCAATTM seeds with gross dislocation densities in the order of 104 cm−2. The photoluminescence spectra of the grown crystals exhibited a predominant near-band-edge emission at 295 K, of which intensity was one order of magnitude higher than the characteristic deep-state emission bands. A nearly bowing-free 60 mm × 60 mm c-plane GaN crystal was eventually obtained.

Plasma-assisted construction of CdO quantum dots/CdS semi-coherent interface for the photocatalytic bio-CO evolution

Heterojunction is promising to promote the spatial charge separation while the poor lattice mismatches and the bulk size of semiconductors constrain the photocarrier separation and migration to the surface. Herein, we report the surface oxidative reconstruction of CdS to form CdO quantum dots (QDs)/CdS intimate heterojunction. We developed a plasma-assisted method to prepare CdO-QDs/CdS heterojunction where CdS(200) and CdO(111) are tilted with a dihedral angel of 159° to form a semi-coherent interface, maximally reducing the interface dangling bonds. The semi-coherent interface and the quantum size of CdO-QDs efficiently promotes charge separation and migration to the surface, accelerating the photocatalytic bio-CO evolution. With glycerol as feedstock, the CO generation rate over CdO-QDs/CdS reaches 2.37 mmol g−1·h−1, which is 4-fold of that over CdS. The present work reports a new method for the preparation of CdO-QDs/CdS intimate heterojunction and gives insight into tuning lattice coherency to promote photocarrier separation.

Attosecond-Resolved Coherent Control of Lattice Vibrations in Thermoelectric SnSe.

Manipulating lattice vibrations is the cornerstone to achieving ultralow thermal conductivity in thermoelectrics. Although spatial control by novel material designs has been recently reported, temporal manipulation, which can shape thermoelectric properties under nonequilibrium conditions, remains largely unexplored. Here, taking SnSe as a representative, we have demonstrated that in the ultrafast pump-pump-probe spectroscopy, electronic and lattice coherences inherited from optical excitations can be exploited independently to manipulate phonon oscillations in a highly selective manner. Specifically, when the pump-pump delay time (tmod) is in the electronic coherence time range, the amplitude, frequency, and lifetime of all phonon modes are simultaneously following the optical cycle. While extending tmod into the lattice coherence time range, the amplitude of each coherent phonon mode can be selectively manipulated according to its intrinsic period without changing the frequency and lifetime. This work opens up exciting avenues to temporally and discriminatorily manipulate phononic processes in thermoelectric materials.

Separation of Kondo lattice coherence from crystal electric field in CeIn3 with Nd substitutions

The ${\mathrm{Ce}}_{m}{\mathrm{M}}_{n}{\mathrm{In}}_{3m+2n}$ $(m=1,2;n=0,1)$ family has been one of the most studied families of heavy fermion compounds. This family has revealed many interesting low-temperature physics phenomena, like quantum critical points, heavy fermion superconductivity, and non-Fermi liquid behavior, when these materials are exposed to pressure, magnetic fields, and/or chemical substitution. Here we provide a thorough investigation of the ${\mathrm{Ce}}_{1\ensuremath{-}x}{\mathrm{Nd}}_{x}{\mathrm{In}}_{3}$ phase diagram through single crystal synthesis, x-ray diffraction, energy-dispersive spectroscopy, magnetic susceptibility, and electrical resistivity measurements. Previous electrical resistivity measurements on ${\mathrm{CeIn}}_{3}$ reveal a broad maximum, ${T}_{\text{max}}\ensuremath{\sim}50$ K, which has been associated with the Kondo lattice coherence crossover and/or the crystal electric field depopulation effect as the $4f$ electrons condense from the high-energy quartet down to the ground state doublet. Our findings show that in the most disordered substitution region, $x=0.4--0.5$, these features disjoin to reveal two distinct broad humps in electrical resistivity measurements. Magnetic susceptibility and electrical resistivity data on ${\mathrm{Ce}}_{1\ensuremath{-}x}{\mathrm{Nd}}_{x}{\mathrm{In}}_{3}$ also reveal the antiferromagnetic ordering competition between ${\mathrm{CeIn}}_{3}$ and ${\mathrm{NdIn}}_{3}$, where the ${T}_{\text{N}}$ of ${\mathrm{CeIn}}_{3}$ is linearly suppressed to a critical concentration of ${x}_{\text{Nd}}\ensuremath{\sim}\phantom{\rule{0.16em}{0ex}}0.6$. This concentration is slightly lower than what was previously reported in nonmagnetically substituted ${\mathrm{Ce}}_{1\ensuremath{-}x}{\mathrm{La}}_{x}{\mathrm{In}}_{3}$. Our magnetic susceptibility measurements and subsequent simulations show that in the ${\mathrm{CeIn}}_{3}$ antiferromagnetic regime, ${x}_{\text{Nd}}\ensuremath{\le}\phantom{\rule{0.16em}{0ex}}0.4$, the Nd ions act as free paramagnets. The large magnitude of the associated paramagnetic response then masks the overlapping antiferromagnetic ordering signature of the Ce ions. Overall our study further sheds light on the underlying crystal electric field and Kondo lattice coherence interactions within the ${\mathrm{Ce}}_{m}{\mathrm{M}}_{n}{\mathrm{In}}_{3m+2n}$ family and could stimulate further studies of these systems via neutron diffraction or under applied pressure.