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Christopher M. Pasco

Publications and source records attributed to Christopher M. Pasco.

3 recordsLinked to original sources

Hysteresis without coexistence: disorder-rounded first-order transitions in a van der Waals magnet

Quenched disorder can profoundly modify phase transitions. In low-dimensional systems, theory predicts that even weak quenched disorder can round the thermodynamic discontinuities associated with a first-order phase transition. Here, we employ time-domain terahertz spectroscopy to investigate the quasi-two-dimensional trimerized kagome van der Waals magnet family Nb$_3$Cl$_{8-x}$Br$_x$ ($x=0$, 1 and 8). We observe the emergence of an additional phonon branch upon Br substitution, whose spectral weight increases and frequency softens with increasing Br concentration. The temperature evolution of the phonon frequencies reveals a clean first-order transition in Nb$_3$Cl$_8$ characterized by macroscopic phase coexistence and thermal hysteresis. In contrast, the transition in the substitutionally disordered compound Nb$_3$Cl$_7$Br retains its hysteresis while exhibiting a substantially broadened transition with no resolvable macroscopic phase coexistence. These observations reveal disorder-induced fragmentation of the transition into locally favored domains instead of well-defined bulk phases separated by stable phase boundaries. The behavior is consistent with the Imry-Wortis and the Aizenman-Wehr scenarios for the effect of quenched disorder in low-dimensional systems, which destabilizes macroscopic phase coexistence and rounds the thermodynamic discontinuities associated with first-order transitions. Thermal hysteresis persists in the disordered compound despite the lack of resolvable coexistence, indicating that the two features often treated as a single hallmark of first-order character arise distinctly and can be separated by disorder. Moreover, our results establish Nb$_3$Cl$_{8-x}$Br$_x$ as a promising platform for investigating the effects of disorder on first-order transitions in low-dimensional systems.

cond-mat.str-el

Magnetism of single crystalline breathing pyrochlore spinel AgInCr4S8

Single crystals of \ce{AgInCr4S8} were grown by chemical vapor transport and crystallographic ordering of Ag/In that results in a breathing pyrochlore motif of Cr$^{3+}$ was verified by x-ray and neutron diffraction. Long-range antiferromagnetic order is observed below a Néel temperature of $T_{\mathrm N}$ $\approx$ 9.6 K. The magnetic properties are characterized using ac and dc magnetization, specific heat capacity, and single crystal neutron diffraction measurements. The specific heat data are characterized by a small lambda anomaly near 9.5 K and the estimated magnetic entropy reaches $\approx$ $\frac{1}{3}$ of the expected value by 3$T_{\mathrm N}$, suggesting significant short-range order in the paramagnetic phase. Single crystal neutron diffraction evidences an incommensurate spin structure with propagation vector $\textbf{\textit{k}}$ = (0,0,$δ$) and $δ$ = 0.343 at 5 K. The minimal model that accounts for the data consists of ferromagnetic layers of Cr atoms, with magnetic moments lying in the plane of the layers and modulating in the perpendicular direction to form a helical structure propagating along $\textbf{\textit{k}}$. This study represents a rare investigation of single crystals within the family of breathing pyrochlore materials.

cond-mat.str-el

Tunable Magnetic Transition to a Singlet Ground State in a 2D Van der Waals Layered Trimerized Kagomé Magnet

Incorporating magnetism into two dimensional (2D) van der Waals (VdW) heterostrutures is crucial for the development of functional electronic and magnetic devices. Here we show that Nb3X8 (X = Cl, Br) is a family of 2D layered trimerized kagomé magnets that are paramagnetic at high temperatures and undergo a first order phase transition on cooling to a singlet magnetic state. X-ray diffraction shows that a rearrangement of the VdW stacking accompanies the magnetic transition, with high and low temperature phases consistent with STEM images of the end members α-Nb3Cl8 and \b{eta}-Nb3Br8. The temperature of this transition is systematically varied across the solid solution Nb3Cl8-xBrx (x = 0-8), with x = 6 having transitions near room temperature. The solid solution also varies the optical properties, which are further modulated by the phase transition. As such, they provide a platform on which to understand and exploit the interplay between dimensionality, magnetism, and optoelectronic behavior in VdW materials.

cond-mat.mtrl-sci