\documentclass[aps,prl,reprint]{revtex4-1} \usepackage[utf8]{inputenc} \usepackage{amsmath,graphicx,upgreek,amssymb} % Our mysterious boy \def\urusi{URu$_2$Si$_2\ $} \def\e{{\mathrm e}} % "elastic" \def\o{{\mathrm o}} % "order parameter" \def\i{{\mathrm i}} % "interaction" \def\Dfh{D$_{4\mathrm h}$} % Irreducible representations (use in math mode) \def\Aog{{\mathrm A_{1\mathrm g}}} \def\Atg{{\mathrm A_{2\mathrm g}}} \def\Bog{{\mathrm B_{1\mathrm g}}} \def\Btg{{\mathrm B_{2\mathrm g}}} \def\Eg {{\mathrm E_{ \mathrm g}}} \def\Aou{{\mathrm A_{1\mathrm u}}} \def\Atu{{\mathrm A_{2\mathrm u}}} \def\Bou{{\mathrm B_{1\mathrm u}}} \def\Btu{{\mathrm B_{2\mathrm u}}} \def\Eu {{\mathrm E_{ \mathrm u}}} % Variables to represent some representation \def\X{\mathrm X} \def\Y{\mathrm Y} % Units \def\J{\mathrm J} \def\m{\mathrm m} \def\K{\mathrm K} \def\GPa{\mathrm{GPa}} \def\A{\mathrm{\c A}} % Other \def\G{\mathrm G} % Ginzburg \begin{document} \title{Elastic properties of \urusi are reproduced by modulated $\Bog$ order} \author{Jaron Kent-Dobias} \author{Michael Matty} \author{Brad Ramshaw} \affiliation{ Laboratory of Atomic \& Solid State Physics, Cornell University, Ithaca, NY, USA } \date\today \begin{abstract} We develop a phenomenological theory for the elastic response of materials with a \Dfh\ point group through phase transitions. The physics is generically that of Lifshitz points, with disordered, uniform ordered, and modulated ordered phases. Several experimental features of \urusi are reproduced when the order parameter has $\Bog$ symmetry: the topology of the temperature--pressure phase diagram, the response of the strain stiffness tensor above the hidden-order transition, and the strain response in the antiferromagnetic phase. In this scenario, the hidden order is a version of the high-pressure antiferromagnetic order modulated along the symmetry axis. \end{abstract} \maketitle \begin{enumerate} \item Introduction \begin{enumerate} \item \urusi hidden order intro paragraph, discuss the phase diagram \item Strain/OP coupling discussion/RUS \item Discussion of experimental data \item We look at MFT's for OP's of various symmetries \end{enumerate} \item Theory \begin{enumerate} \item Introduce various pieces of free energy \item Summary of MFT results \end{enumerate} \item Data piece \item Talk about more cool stuff like AFM C4 breaking etc \end{enumerate} The study of phase transitions is a central theme of condensed matter physics. In many cases, a phase transition between different states of matter is marked by a change in symmetry. In this paradigm, the breaking of symmetry in an ordered phase corresponds to the condensation of an order parameter (OP) that breaks the same symmetries. Near a second order phase transition, the physics of the OP can often be described in the context of Landau-Ginzburg mean field theory. However, to construct such a theory, one must know the symmetries of the order parameter, i.e. the symmetry of the ordered state. One quintessential case where the symmetry of an ordered phase remains unknown is in \urusi. \urusi is a heavy fermion superconductor in which superconductivity condenses out of a symmetry broken state referred to as hidden order (HO) [cite pd paper], and at sufficiently large [hydrostatic?] pressures, both give way to local moment antiferromagnetism. Despite over thirty years of effort, the symmetry of the hidden order state remains unknown, and modern theories [big citation chunk] propose a variety of possibilities. Many [all?] of these theories rely on the formulation of a microscopic model for the HO state, but without direct experimental observation of the broken symmetry, none have been confirmed. One case that does not rely on a microscopic model is recent work [cite RUS paper] that studies the HO transition using resonant ultrasound spectroscopy (RUS). RUS is an experimental technique that measures mechanical resonances of a sample. These resonances contain information about the full elastic tensor of the material. Moreover, the frequency locations of the resonances are sensitive to symmetry breaking at an electronic phase transition due to electron-phonon coupling [cite]. Ref. [RUS paper] uses this information to place strict thermodynamic bounds on the symmetry of the HO OP, again, independent of any microscopic model. Motivated by these results, in this paper we consider a mean field theory of an OP coupled to strain and the effect that the OP symmetry has on the elastic response in different symmetry channels. Our study finds that a single possible OP symmetry reproduces the experimental strain susceptibilities, and fits the experimental data well. The point group of \urusi is \Dfh, and any coarse-grained theory must locally respect this symmetry. We will introduce a phenomenological free energy density in three parts: that of the strain, the order parameter, and their interaction. The most general quadratic free energy of the strain $\epsilon$ is $f_\e=\lambda_{ijkl}\epsilon_{ij}\epsilon_{kl}$, but the form of the $\lambda$ tensor is constrained by both that $\epsilon$ is a symmetric tensor and by the point group symmetry \cite{landau_theory_1995}. The latter can be seen in a systematic way. First, the six independent components of strain are written as linear combinations that behave like irreducible representations under the action of the point group, or \begin{equation} \begin{aligned} \epsilon_\Aog^{(1)}=\epsilon_{11}+\epsilon_{22} && \hspace{0.1\columnwidth} \epsilon_\Aog^{(2)}=\epsilon_{33} \\ \epsilon_\Bog^{(1)}=\epsilon_{11}-\epsilon_{22} && \epsilon_\Btg^{(1)}=2\epsilon_{12} \\ \epsilon_\Eg^{(1)}=2\{\epsilon_{11},\epsilon_{22}\}. \end{aligned} \end{equation} Next, all quadratic combinations of these irreducible strains that transform like $\Aog$ are included in the free energy as \begin{equation} f_\e=\frac12\sum_\X\lambda_\X^{(ij)}\epsilon_\X^{(i)}\epsilon_\X^{(j)}, \end{equation} where the sum is over irreducible representations of the point group and the stiffnesses $\lambda_\X^{(ij)}$ are \begin{equation} \begin{aligned} &\lambda_{\Aog}^{(11)}=\tfrac12(\lambda_{1111}+\lambda_{1122}) && \lambda_{\Aog}^{(22)}=\lambda_{3333} \\ &\lambda_{\Aog}^{(12)}=\lambda_{1133} && \lambda_{\Bog}^{(11)}=\tfrac12(\lambda_{1111}-\lambda_{1122}) \\ &\lambda_{\Btg}^{(11)}=\lambda_{1212} && \lambda_{\Eg}^{(11)}=\lambda_{1313}. \end{aligned} \end{equation} The interaction between strain and the order parameter $\eta$ depends on the representation of the point group that $\eta$ transforms as. If this representation is $\X$, then the most general coupling to linear order is \begin{equation} f_\i=b^{(i)}\epsilon_\X^{(i)}\eta \end{equation} If $\X$ is a representation not present in the strain there can be no linear coupling, and the effect of $\eta$ going through a continuous phase transition is to produce a jump in the $\Aog$ strain stiffness. We will therefore focus our attention on order parameter symmetries that produce linear couplings to strain. If the order parameter transforms like $\Aog$, odd terms are allowed in its free energy and any transition will be abrupt and not continuous without tuning. For $\X$ as any of $\Bog$, $\Btg$, or $\Eg$, the most general quartic free energy density is \begin{equation} \begin{aligned} f_\o=\frac12\big[&r\eta^2+c_\parallel(\nabla_\parallel\eta)^2 +c_\perp(\nabla_\perp\eta)^2 \\ &\quad+D_\parallel(\nabla_\parallel^2\eta)^2 +D_\perp(\nabla_\perp^2\eta)^2\big]+u\eta^4 \end{aligned} \label{eq:fo} \end{equation} where $\nabla_\parallel=\{\partial_1,\partial_2\}$ transforms like $\Eu$ and $\nabla_\perp=\partial_3$ transforms like $\Atu$. We'll take $D_\parallel=0$ since this does not affect the physics at hand. Neglecting interaction terms higher than quadratic order, the only strain relevant to the problem is $\epsilon_\X$, and this can be traced out of the problem exactly, since \begin{equation} 0=\frac{\delta F}{\delta\epsilon_{\X i}(x)}=\lambda_\X\epsilon_{\X i}(x) +\frac12b\eta_i(x) \end{equation} gives $\epsilon_\X(x)=-(b/2\lambda_\X)\eta(x)$. Upon substitution into the free energy, tracing out $\epsilon_\X$ has the effect of shifting $r$ in $f_\o$, with $r\to\tilde r=r-b^2/4\lambda_\X$. With the strain traced out \eqref{eq:fo} describes the theory of a Lifshitz point at $\tilde r=c_\perp=0$ \cite{lifshitz_theory_1942, lifshitz_theory_1942-1}. For a scalar order parameter ($\Bog$ or $\Btg$) it is traditional to make the field ansatz $\eta(x)=\eta_*\cos(q_*x_3)$. For $\tilde r>0$ and $c_\perp>0$, or $\tilde r0$, and the modulated phase is now characterized by helical order with $\eta(x)=\eta_*\{\cos(q_*x_3),\sin(q_*x_3)\}$ and \begin{equation} \eta_*^2=\frac{c_\perp^2-4D_\perp\tilde r}{16D_\perp u} =\frac{\tilde r_c-\tilde r}{4u} \end{equation} The uniform--modulated transition is now continuous. The schematic phase diagrams for this model are shown in Figure \ref{fig:phases}. \begin{figure}[htpb] \includegraphics[width=0.51\columnwidth]{phases_scalar}\hspace{-1.5em} \includegraphics[width=0.51\columnwidth]{phases_vector} \caption{ Schematic phase diagrams for this model. Solid lines denote continuous transitions, while dashed lines indicated abrupt transitions. (a) The phases for a scalar ($\Bog$ or $\Btg$). (b) The phases for a vector ($\Eg$). } \label{fig:phases} \end{figure} The susceptibility is given by \begin{equation} \begin{aligned} &\chi_{ij}^{-1}(x,x') =\frac{\delta^2F}{\delta\eta_i(x)\delta\eta_j(x')} \\ &\quad=\Big[\big(\tilde r-c_\parallel\nabla_\parallel^2 -c_\perp\nabla_\perp^2+D_\perp\nabla_\perp^4+4u\eta^2(x)\big)\delta_{ij} \\ &\qquad\qquad +8u\eta_i(x)\eta_j(x)\Big]\delta(x-x'), \end{aligned} \end{equation} or in Fourier space, \begin{equation} \begin{aligned} \chi_{ij}^{-1}(q) &=8u\sum_{q'}\tilde\eta_i(q')\eta_j(-q')+\bigg(\tilde r +c_\parallel q_\parallel^2-c_\perp q_\perp^2 \\ &\qquad+D_\perp q_\perp^4+4u\sum_{q'}\tilde\eta_k(q')\tilde\eta_k(-q')\bigg) \delta_{ij}. \end{aligned} \end{equation} Near the unordered--modulated transition this yields \begin{equation} \begin{aligned} \chi_{ij}(q) &=\frac{\delta_{ij}}{c_\parallel q_\parallel^2+D_\perp(q_*^2-q_\perp^2)^2 +|\tilde r-\tilde r_c|} \\ &=\frac{\delta_{ij}}{D_\perp}\frac{\xi_\perp^4} {1+\xi_\parallel^2q_\parallel^2+\xi_\perp^4(q_*^2-q_\perp^2)^2}, \end{aligned} \label{eq:susceptibility} \end{equation} with $\xi_\perp=(|\tilde r-\tilde r_c|/D_\perp)^{-1/4}$ and $\xi_\parallel=(|\tilde r-\tilde r_c|/c_\parallel)^{-1/2}$. The elastic susceptibility (inverse stiffness) is given in the same way: we must trace over $\eta$ and take the second variation of the resulting free energy. Extremizing over $\eta$ yields \begin{equation} 0=\frac{\delta F}{\delta\eta_i(x)}=\frac{\delta F_\o}{\delta\eta_i(x)} +\frac12b\epsilon_{\X i}(x), \label{eq:implicit.eta} \end{equation} which implicitly gives $\eta$ as a functional of $\epsilon_\X$. Though this cannot be solved explicitly, we can make use of the inverse function theorem to write \begin{equation} \begin{aligned} \bigg(\frac{\delta\eta_i(x)}{\delta\epsilon_{\X j}(x')}\bigg)^{-1} &=\frac{\delta\eta_j^{-1}[\eta](x)}{\delta\eta_i(x')} =-\frac2b\frac{\delta^2F_\o}{\delta\eta_i(x)\delta\eta_j(x')} \\ &=-\frac2b\chi_{ij}^{-1}(x,x')-\frac{b}{2\lambda_\X}\delta_{ij}\delta(x-x') \end{aligned} \label{eq:inv.func} \end{equation} It follows from \eqref{eq:implicit.eta} and \eqref{eq:inv.func} that the susceptibility of the material to $\epsilon_\X$ strain is given by \begin{widetext} \begin{equation} \begin{aligned} \chi_{\X ij}^{-1}(x,x') &=\frac{\delta^2F}{\delta\epsilon_{\X i}(x)\delta\epsilon_{\X j}(x')} \\ &=\lambda_\X\delta_{ij}\delta(x-x')+ b\frac{\delta\eta_i(x)}{\delta\epsilon_{\X j}(x')} +\frac12b\int dx''\,\epsilon_{\X k}(x'')\frac{\delta^2\eta_k(x)}{\delta\epsilon_{\X i}(x')\delta\epsilon_{\X j}(x'')} \\ &\qquad+\int dx''\,dx'''\,\frac{\delta^2F_\o}{\delta\eta_k(x'')\delta\eta_\ell(x''')}\frac{\delta\eta_k(x'')}{\delta\epsilon_{\X i}(x)}\frac{\delta\eta_\ell(x''')}{\delta\epsilon_{\X j}(x')} +\int dx''\,\frac{\delta F_\o}{\delta\eta_k(x'')}\frac{\delta\eta_k(x'')}{\delta\epsilon_{\X i}(x)\delta\epsilon_{\X j}(x')} \\ &=\lambda_\X\delta_{ij}\delta(x-x')+ b\frac{\delta\eta_i(x)}{\delta\epsilon_{\X j}(x')} -\frac12b\int dx''\,dx'''\,\bigg(\frac{\partial\eta_k(x'')}{\partial\epsilon_{\X\ell}(x''')}\bigg)^{-1}\frac{\delta\eta_k(x'')}{\delta\epsilon_{\X i}(x)}\frac{\delta\eta_\ell(x''')}{\delta\epsilon_{\X j}(x')} \\ &=\lambda_\X\delta_{ij}\delta(x-x')+ b\frac{\delta\eta_i(x)}{\delta\epsilon_{\X j}(x')} -\frac12b\int dx''\,\delta_{i\ell}\delta(x-x'')\frac{\delta\eta_\ell(x'')}{\delta\epsilon_{\X j}(x')} =\lambda_\X\delta_{ij}\delta(x-x')+ \frac12b\frac{\delta\eta_i(x)}{\delta\epsilon_{\X j}(x')}, \end{aligned} \end{equation} \end{widetext} whose Fourier transform follows from \eqref{eq:inv.func} as \begin{equation} \chi_{\X ij}(q)=\frac{\delta_{ij}}{\lambda_\X}+\frac{b^2}{4\lambda_\X^2}\chi_{ij}(q). \label{eq:elastic.susceptibility} \end{equation} At $q=0$, which is where the stiffness measurements used here were taken, this predicts a cusp in the elastic susceptibility of the form $|\tilde r-\tilde r_c|^\gamma$ for $\gamma=1$. \begin{figure}[htpb] \centering \includegraphics[width=\columnwidth]{fig-stiffnesses} \caption{ Measurements of the effective strain stiffness as a function of temperature for the six independent components of strain from ultrasound. The vertical dashed lines show the location of the hidden order transition. } \label{fig:data} \end{figure} We have seen that mean field theory predicts that whatever component of strain transforms like the order parameter will see a $t^{-1}$ softening in the stiffness that ends in a cusp. Ultrasound experiments \textbf{[Elaborate???]} yield the strain stiffness for various components of the strain; this data is shown in Figure \ref{fig:data}. The $\Btg$ and $\Eg$ stiffnesses don't appear to have any response to the presence of the transition, exhibiting the expected linear stiffening with a low-temperature cutoff \textbf{[What's this called? Citation?]}. The $\Bog$ stiffness has a dramatic response, softening over the course of roughly $100\,\K$. There is a kink in the curve right at the transition. While the low-temperature response is not as dramatic as the theory predicts, mean field theory---which is based on a small-$\eta$ expansion---will not work quantitatively far below the transition where $\eta$ has a large nonzero value and higher powers in the free energy become important. The data in the high-temperature phase can be fit to the theory \eqref{eq:elastic.susceptibility}, with a linear background stiffness $\lambda_\Bog^{(11)}$ and $\tilde r-\tilde r_c=a(T-T_c)$, and the result is shown in Figure \ref{fig:fit}. The data and theory appear consistent. \begin{figure}[htpb] \includegraphics[width=\columnwidth]{fig-fit} \caption{ Strain stiffness data for the $\Bog$ component of strain (solid) along with a fit of \eqref{eq:elastic.susceptibility} to the data above $T_c$ (dashed). The fit gives $\lambda_\Bog^{(11)}\simeq\big[71-(0.010\,\K^{-1})T\big]\,\GPa$, $b^2/4D_\perp q_*^4\simeq6.2\,\GPa$, and $a/D_\perp q_*^4\simeq0.0038\,\K^{-1}$. } \label{fig:fit} \end{figure} Mean field theory neglects the effect of fluctuations on critical behavior, yet also predicts the magnitude of those fluctuations. This allows a mean field theory to undergo an internal consistency check to ensure the predicted fluctuations are indeed negligible. This is typically done by computing the Ginzburg criterion \cite{ginzburg_remarks_1961}, which gives the proximity to the critical point $t=(T-T_c)/T_c$ at which mean field theory is expected to break down by comparing the magnitude of fluctuations in a correlation-length sized box to the magnitude of the field, or since the correlation function is $k_BT\chi(x,x')$, \begin{equation} V_\xi^{-1}k_BT\int_{V_\xi}d^3x\,\chi(x,0) =\langle\delta\eta^2\rangle_{V_\xi} \lesssim\frac12\eta_*^2=\frac{|\Delta\tilde r|}{6u} \end{equation} with $V_\xi$ the correlation volume, which we will take to be a cylinder of radius $\xi_\parallel/2$ and height $\xi_\perp$. Upon substitution of \eqref{eq:susceptibility} and using the jump in the specific heat at the transition from \begin{equation} c_V=-T\frac{\partial^2f}{\partial T^2} =\begin{cases}0&T>T_c\\Ta^2/12 u&T1\,\K$, and so it remains self-consistent. \begin{acknowledgements} \end{acknowledgements} \bibliography{hidden_order} \end{document}