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# Spin Correlations and Magnetic Order in Nonsuperconducting Nd2-xCexCuO4±δ

## Abstract

We report quantitative neutron scattering measurements of the evolution with doping of the Néel temperature, the antiferromagnetic correlations, and the ordered moment of as-grown, non-superconducting Nd2-xCexCuO4±δ ($`0x0.18`$). The instantaneous correlation length can be effectively described by our quantum Monte Carlo calculations for the randomly site-diluted nearest-neighbor spin-1/2 square-lattice Heisenberg antiferromagnet. However, quantum fluctuations have a stronger effect on the ordered moment, which decreases more rapidly than for the quenched-disorder model.

Over the past eighteen years much has been learned about the evolution with doping of magnetic correlations in the high-temperature superconductors. For the prototypical material La2-xSrxCuO4 (LSCO), neutron scattering has led to the observation of the loss of long-range antiferromagnetic order and the concomitant decrease of two-dimensional (2D) spin correlations LSC , an incommensurate spin-density wave yam , and coupled charge and magnetic “stripe” order upon codoping with Nd tra (a). The richness of the observed behavior is attributable to the evolution of the cuprate superconductors from Mott-insulating parent materials which are found to be excellent realizations, at low energies and long wavelengths, of the spin-1/2 square-lattice Heisenberg antiferromagnet (SLHAF) bir . Although the vast majority of research has focused on the hole-doped systems, the electron-doped materials, typified by Nd2-xCexCuO4±δ (NCCO) Tokura et al. (1989), have presented an important challenge to the field of high-$`T_\mathrm{c}`$ research and particularly to the paradigm established from experiments on LSCO. Unlike for LSCO, the magnetic phase of NCCO is very robust with respect to doping luk ; thu ; mat  and the magnetic correlations remain commensurate mat ; Yamada et al. (1999).

Since superconductivity in the high-$`T_\mathrm{c}`$ cuprates appears in close proximity to antiferromagnetic phases, it is essential to understand the nature of nearby magnetic ground states. As-grown, NCCO is not superconducting, and the antiferromagnetic phase extends to the highest concentration for which samples can be produced ($`x0.18`$). Oxygen impurities are believed to occupy the nominally vacant apical sites Schultz et al. (1996), and a relatively severe oxygen reduction procedure must be applied to induce superconductivity above $`x=0.13`$ Tokura et al. (1989). Although the reduction procedure weakens the magnetism, magnetic order is still observed near optimal doping where $`T_\mathrm{c}=24`$ K mat ; uef . One qualitative argument often employed to explain the robustness of the antiferromagnetic phase in the electron-doped cuprates is that, whereas hole carriers are doped into the O 2p band and frustrate the antiferromagnetic arrangement of the neighboring Cu ions, doped electrons primarily reside on the Cu site, filling the 3d shell and removing the spin degree of freedom luk ; thu ; mat . New, quantitative insights have been gained recently into the role of $`static`$ non-magnetic impurities introduced into the spin-1/2 SLHAF Sachdev et al. (1999); Sandvik (2002); vaj ; bil , and it would be interesting to test how well NCCO can be described by this model.

In this Letter, we present detailed neutron scattering results on the evolution with Ce doping of the magnetic properties of as-grown, non-superconducting Nd2-xCexCuO4±δ ($`0x0.18`$). We find that the instantaneous spin correlations in the paramagnetic phase are, in effect, well described by the randomly-diluted spin-1/2 nearest-neighbor (NN) SLHAF model for which we have carried out numerical simulations. On the other hand, the ordered moment falls off more rapidly, a clear indication that quantum fluctuations are stronger than for the model magnet and that such fluctuations manifest themselves differently for different observables. We also find that the primary difference between the Néel temperature and ordered moment of as-grown and reduced NCCO is a shift in electron concentration that corresponds to $`|\mathrm{\Delta }x|0.03`$.

Crystals of Nd2-xCexCuO4±δ were grown in 4 atm of O2 using the traveling-solvent floating-zone technique. The solubility limit is about $`x=0.18`$, and our study spans the range $`0x0.18`$. In addition, several samples were reduced for 20 h at 960C in Ar, followed by an anneal for 20 h at 500C in O2, for additional magnetic order parameter measurements. Magnetometry indicates that the reduced $`x=0.14`$ and $`x=0.18`$ samples are superconducting with $`T_\mathrm{c}=24`$ and 20 K (onset), respectively. Our single-grain crystals are cylindrical, typically with a diameter of 4.5 mm, and range in volume from 0.1 to 0.7 cm3. Average Ce concentrations were verified using inductively coupled plasma spectroscopy and typically found to equal the nominal values. The neutron scattering measurements were performed on the thermal triple-axis instruments BT2 and BT9 of the National Institute of Standards and Technology Center for Neutron Research.

All as-grown samples exhibit long-range magnetic order at low temperature. However, significant two-dimensional (2D) magnetic correlations are already present well above the Néel temperature mat . These may be probed through “two-axis” scans in which one integrates the dynamic structure factor $`S(\text{q}_{2\mathrm{D}},\omega )`$ over the limits set by the thermal energy, $`k_\text{B}T`$, and the incident neutron energy, $`E_i`$. If the integration is carried out over the relevant fluctuations one obtains the equal-time structure factor $`S(\text{q}_{2\mathrm{D}})`$ bir . In Fig. 1, we present representative scans of this type that show a peak in $`S(\text{q}_{2\mathrm{D}})`$ at the incipient antiferromagnetic ordering wavevector. We fit these data to an isotropic 2D Lorentzian, $`S(q_{2\mathrm{D}})=S(0)/(1+q_{2\mathrm{D}}^2\xi ^2)`$, convolved with the instrumental resolution. As the temperature or the doping level is increased, the correlation length $`\xi `$ decreases, which manifests itself as a broadening of the peaks.

Figure 2 summarizes the behavior of $`\xi (x,T)`$ for several Ce concentrations. Over a wide temperature range, the spin correlations exhibit an exponential dependence on inverse temperature, $`\xi (x,T)\mathrm{exp}[2\pi \rho _s(x)/T]`$ with spin stiffness $`\rho _\mathrm{s}(x)`$, indicative of an underlying ground state with 2D antiferromagnetic order Chakravarty et al. (1989). We overlay the results of quantum Monte Carlo simulations for the randomly-diluted SLHAF, described by the Hamiltonian

$$=J\underset{i,j}{}p_ip_j𝐒_i𝐒_j,$$
(1)
where the sum is over NN sites, $`J`$ is the antiferromagnetic Cu-O-Cu superexchange, $`𝐒_i`$ is the spin-1/2 operator at site i, $`p_i=1`$ on magnetic sites, and $`p_i=0`$ on nonmagnetic sites. The numerical method is the same as that employed previously vaj . The data are plotted as $`\xi /a`$, the ratio of the spin-spin correlation length to the NN Cu-Cu distance ($`a3.95`$ Å), versus $`J/T`$, the ratio of the NN antiferromagnetic superexchange of Nd2CuO4 to the temperature. A previous estimate from comparison of $`\xi (T)`$ with theory for the SLHAF yielded $`J130`$ meV thu , and we find $`J=125(4)`$ meV from comparison with our numerical results for $`x=0`$. Since the value of $`J`$ has been established, the only adjustable parameter in the comparison for the Ce-doped samples is the concentration of nonmagnetic sites in Eq. (1). We find good qualitative agreement between experiment and Monte Carlo if we fix this concentration to equal the nominal Ce concentration $`x`$. However, as shown in Fig. 2, the agreement becomes quantitative if we allow the effective dilution to differ slightly: $`x_{\mathrm{eff}}(x=0.10)=0.08(1)`$, $`x_{\mathrm{eff}}(x=0.14)=0.12(1)`$, and $`x_{\mathrm{eff}}(x=0.18)=0.21(2)`$. Also shown are previous data for as-grown samples with $`x=0`$ and $`x=0.15`$ thu ; mat . The result for Nd2CuO4 agrees well with ours, and we estimate that $`x_{\mathrm{eff}}(x=0.15)=0.16(2)`$. The extent to which the quenched-disorder model Eq. (1) effectively describes the spin correlations of as-grown, non-superconducting NCCO is remarkable. The observed small differences between nominal electron concentration and effective static dilution may be in part due to the uncertainty in the oxygen (and hence electron) concentration of our samples. Another likely possibility is the presence of additional quantum fluctuations which are not captured in the effective Hamiltonian Eq. (1), for example due to frustrating next-NN interactions.

The spin stiffness of the disorder-free spin-1/2 NN SLHAF is known to be $`2\pi \rho _\mathrm{s}/J=1.131(3)`$ Beard et al. (1998). An estimate for the case of quenched disorder, Eq. (1), has been obtained in previous numerical work vaj . Comparison of the experimental results in Fig. 2 gives the effective values $`2\pi \rho _\mathrm{s}/J=0.71(2)`$, 0.54(4), 0.40(7), and 0.25(5), respectively, for $`x=0.10`$, 0.14, 0.15, and 0.18. The value 0.40(7) for the $`x=0.15`$ sample is somewhat smaller than the original estimate of $`2\pi \rho _\mathrm{s}/J0.54`$ mat  which was based on a classical rather than a quantum vaj  picture for the doping dependence of the spin stiffness.

We note that Ref. mat  reports data for two as-grown $`x=0.15`$ samples with onset of magnetic order at $`T_\mathrm{N}=160`$ and 125 K. If we allow for a distribution of Néel temperatures to account for the rounding of the observed transition, we estimate mean values of $`T_\mathrm{N}=147(17)`$ and 115(9) K, respectively. This is consistent with how we have treated our own data. The second sample from Ref. mat  also exhibits lower values of $`\xi (T)`$ (not shown in Fig. 2), comparable to our $`x=0.18`$ crystal. The removal of oxygens through the reduction process changes both the degree of disorder and the carrier concentration. This lowers the Néel temperature and, for $`x>0.13`$, leads to a decrease of the antiferromagnetic volume fraction and to bulk superconductivity uef . Growth at lower oxygen partial pressure mimics the reduction process, resulting in lower oxygen contents and higher effective doping levels. The primary focus of this Letter is on non-superconducting, as-grown NCCO, and therefore we were careful to grow our samples under high oxygen partial pressure, resulting in crystals with $`T_\mathrm{N}`$ at or close to the maximum value attainable.

Figure 3(a) indicates that the Néel temperature $`T_\mathrm{N}(x)`$ of our as-grown samples, as obtained from neutron diffraction, approximately follows a parabolic form, extrapolating to zero at $`x0.21`$. As shown in Fig. 3(a), qualitatively similar behavior was found previously for reduced NCCO for which $`T_\mathrm{N}(x)`$ is lower Uefuji et al. (2002). The primary effect of the reduction is an approximately rigid shift by $`|\mathrm{\Delta }x|0.03`$ due to the change in carrier density. The concave doping dependence for NCCO is contrasted by the behavior exhibited by the randomly-diluted spin-1/2 SLHAF La2Cu1-x(Zn,Mg)xO4 (LCZMO), for which Néel order extends up to the site percolation threshold, $`x_\mathrm{p}0.41,`$ and the 2D spin correlations are quantitatively described by Eq. (1) up to $`x_\mathrm{p}`$ vaj .

In Fig. 3(b), we plot the ordered moment for several samples, as obtained from order parameter measurements at low temperature. The values are normalized to that of Nd2CuO4. Consistent with the behavior of $`T_\mathrm{N}(x)`$, the ordered moment of as-grown NCCO approaches zero much more rapidly than in the case of random dilution: at the rate $`1M_{\mathrm{st}}(x)/M_{\mathrm{st}}(0)3.5x`$ which is approximately twice that of the diluted spin-1/2 SLHAF for $`x<0.20.`$ On the other hand, the magnetic phase extends much further than for LSCO LSC  and Li-doped La2CuO4 sas , for which Néel order is destroyed above $`x0.02`$ and $`x0.03`$, respectively. The ordered moment of reduced samples is lowered further. We note that these data are again normalized by the value for as-grown Nd2CuO4, and that a rigid shift of $`|\mathrm{\Delta }x|=0.03`$ leads to a good agreement of the two data sets. Our result is consistent with previous experimental work at lower concentrations Rosseinsky et al. (1991).

If viewed instantaneously, so as to mitigate the effects due to the increased itinerancy upon doping, the magnetism of NCCO should indeed resemble a system with quenched random site dilution. What is surprising is that for $`\xi (x,T)`$ the correspondence with Eq. (1) is nearly quantitative. Since the charge carriers in as-grown NCCO are itinerant, even well below $`T_\mathrm{N}`$ tra (b), deviations from the static model Eq. (1) may be expected to emerge as we view the two systems on different time scales. Indeed, the ordered moment, a measure of the strength of the magnetic order at infinitely long times, decreases much more rapidly in the case of NCCO than for the SLHAF. We note that slight deviations, possibly due to the presence of a frustrating next-NN exchange, are already observable for the ordered moment of LCZMO vaj  \[Fig. 3(b)\], and that LCZMO appears to be in close proximity to a new quantum critical point in an extended parameter space bil . In the case of LCZMO, these perturbations are not quite strong enough to shift the critical point away from the geometric site-percolation threshold. Although the experimentally accessible doping range is limited, our results for NCCO are consistent with the existence of a quantum critical point below the geometric site-percolation threshold.

We note that recent calculations for the one-band Hubbard model are in semi-quantitative agreement with our data for the spin correlations mar ; kyu  and ordered moment mar ; kus ; bob . The latter result is shown in Fig. 3(b). These theories were motivated by photoemission measurements of the evolution of the Fermi surface of reduced Nd2-xCexCuO4±δ ($`0x0.15`$) arm . Their proponents assert that t–J models are intrinsically limited in describing the electron-doped cuprates and that a proper description requires t–U models with a decreasing value of $`U`$ with increasing electron concentration kus ; mar ; sen ; kyu .

In summary, we have presented a comprehensive neutron scattering study of the magnetic properties of non-superconducting Nd2-xCexCuO4±δ. Although the evolution of the instantaneous spin-correlations may effectively be described by a site-dilution model, a proper description of the magnetic degrees of freedom must necessarily include the effects of electron itinerancy. While the achievements of recent theoretical treatments of the Hubbard model seem very promising, it is not clear at present if this model exhibits a superconducting ground state. Phonon anomalies have been observed in both electron and hole doped high-temperature superconductors das , and a complete description of these materials may require the additional consideration of the electron-lattice coupling. Regardless, our data should serve as a benchmark for tests of still-emerging theories for the high-$`T_\mathrm{c}`$ phase diagram.

We acknowledge valuable discussions with N.P. Armitage, S. Larochelle, R.S. Markiewicz, M. Matsuda, and A.-M. S. Tremblay, and thank I. Tanaka and the late H. Kojima for their invaluable assistance during the initial stage of the crystal growth effort. This work was supported by the US Department of Energy under Contracts No. DE-FG03-99ER45773 and No. DE-AC03-76SF00515, and by NSF CAREER Award No. DMR9985067.


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# Spin oscillations in transient diffusion of a spin pulse in 𝑛-type semiconductor quantum wells

thanks: Author to whom correspondence should be addressed

## Abstract

By studying the time and spatial evolution of a spin-polarized pulse in $`n`$-type semiconductor quantum wells, we highlight the importance of the off-diagonal spin coherence in spin diffusion and transport. Spin oscillations and spin polarization reverse along the the direction of spin diffusion in the absence of the applied magnetic field are predicted from our investigation.

There are growing numbers of experimental and theoretical investigations on spin related phenomena due to potential applications in semiconductor spintronic devices such as spin filters and spin transistors.Wolf (2000); Ziese and Thornton (2001); Folk et al. (2003); Zhou et al. (2004); Datta and Das (1990); Johnson (1993); Monsma et al. (1998) An important prerequisite for the realization of such devices is to understand how the spin-polarized electrons transport from one position to another. In experiment, coherent spin propagation over a long distance has been reported.Kikkawa and Awschalom (1998) Spin injections from ferromagnetic materials into semiconductors have been extensively investigated.Hanbicki et al. (2003) In theory most works are based on the quasi-independent electron model and are focused on the diffusive transport regimeZiese and Thornton (2001); Schmidt et al. (2000) in which the spin polarization of the current is controlled by the longitudinal spin dephasing through a relaxation time approximation. There are some efforts on investigating the spin dephasing in the spin transport: Takahashi et al. calculated the spin diffusion coefficients by solving the kinetic equations with only the electron-electron scattering.Takahashi et al. (1999) Bournel et al.Bournel et al. (1997) and Saikin et al.Saikin et al. (2003) studied the spin transport in semiconductor heterostructures with the Rashba effect and the electron-phonon scattering by Monte Carlo simulation. However, in these investigations either the off-diagonal inter-spin-band correlations $`\rho _{𝐤\sigma \sigma }=c_{𝐤\sigma }^{}c_{𝐤\sigma }`$ are discarded (or not explicitly included) or the spin dephasing is simply introduced through the relaxation time approximation.

Recently we performed a many-body investigation of spin transport in GaAs (100) quantum wells (QW’s) by self-consistently solving the many-body kinetic transport equations together with the Poission equation. We have explicitly taken into account the spatial inhomogeneity, the D’yakonov-Perel’ (DP) mechanism and all scattering.Weng and Wu (2002) In our theory, both the diagonal intra-spin-band correlations, i.e., the electron distribution function $`f_{𝐤\sigma }=c_{𝐤\sigma }^{}c_{𝐤\sigma }`$, and the off-diagonal inter-spin-band correlations $`\rho _{𝐤\sigma \sigma }`$ are explicitly included. The spin dephasing time, the spin/charge diffusion length together with the mobility are calculated self-consistently. We further pointed out a novel spin dephasing mechanism in the spin diffusion/transport that the inhomogeneous broadening due to the interference between the electrons/spins with different momenta along the direction of the diffusion can cause spin dephasing in the presence of the scattering and the resulting dephasing can be more important than the dephasing due to the DP mechanism. In this paper, we further investigate the time evolution of a spin-polarized pulse (SPP) in $`n`$-type GaAs (100) QW through the many-body kinetic Bloch equations. We highlight the importance of the off-diagonal spin correlations in the spin diffusion and transport.

In $`n`$-type GaAs QW’s, the dominant spin dephasing mechanism is the DP mechanism.D’yakonov and Perel’ (1971); Meier and Zakharchenya (1984) By taking account of the DP term, the kinetic Bloch equations can be written as

$$\frac{\rho (𝐑,𝐤,t)}{t}\frac{1}{2}\{_𝐑\overline{\epsilon }(𝐑,𝐤,t),_𝐤\rho (𝐑,𝐤,t)\}+\frac{1}{2}\{_𝐤\overline{\epsilon }(𝐑,𝐤,t),_𝐑\rho (𝐑,𝐤,t)\}\frac{\rho (𝐑,𝐤,t)}{t}|_c=\frac{\rho (𝐑,𝐤,t)}{t}|_s.$$

Here $`\rho (𝐑,𝐤,t)`$ represents a single particle density matrix. The diagonal elements describe the electron distribution functions $`\rho _{\sigma \sigma }(𝐑,𝐤,t)=f_\sigma (𝐑,𝐤,t)`$ of wave vector $`𝐤`$ and spin $`\sigma `$($`=\pm 1/2`$) at position $`𝐑`$ and time $`t`$. The off-diagonal elements $`\rho _{\sigma \sigma }(𝐑,𝐤,t)`$ describe the inter-spin-band correlations (coherences) for the spin coherence. The quasi-particle energy $`\overline{\epsilon }_{\sigma \sigma ^{}}(𝐑,𝐤,t)`$, in the presence of a moderate magnetic field $`𝐁`$ and with the DP termD’yakonov and Perel’ (1971) included, reads $`\overline{\epsilon }_{\sigma \sigma ^{}}(𝐑,𝐤,t)=\epsilon _k\delta _{\sigma \sigma ^{}}+\left[g\mu _B𝐁+𝐡(𝐤)\right]𝝈_{\sigma \sigma ^{}}/2e\psi (𝐑,t)+\mathrm{\Sigma }_{\sigma \sigma ^{}}(𝐑,𝐤,t)`$, where $`\epsilon _k=k^2/2m^{}`$ is the energy spectrum with $`m^{}`$ denoting the electron effective mass. $`𝝈`$ are the Pauli matrices. $`𝐡(𝐤)`$ denotes the effective magnetic field from the DP effect which contains contributions from both the DresselhausDresselhaus (1955) term and the Rashba term.Bychkov and Rashba (1984) In this paper, we only consider the Dresselhaus term which can be written asEppenga and Schuurmans (1988) $`h_x(𝐤)=\gamma k_x(k_y^2\kappa _z^2)`$ and $`h_y(𝐤)=\gamma k_y(\kappa _z^2k_x^2)`$ with $`\gamma `$ denoting the spin-orbit coupling strengthAronov et al. (1983) and $`\kappa _z^2`$ representing the average of the operator $`(/z)^2`$ over the electronic state of the lowest subband. The electric potential $`\psi (𝐑,t)`$ satisfies the Poission equation

$$_𝐑^2\psi (𝐑,t)=e\left[n(𝐑,t)n_0(𝐑)\right]/ϵ,$$
(1)
where $`n(𝐑,t)=_{\sigma 𝐤}f_\sigma (𝐑,𝐤,t)`$ is the electron density at position $`𝐑`$ and time $`t`$ and $`n_0(𝐑)`$ is the positive background electric charge density. $`\mathrm{\Sigma }_{\sigma \sigma ^{}}(𝐑,𝐤,t)=_𝐪V_𝐪\rho _{\sigma \sigma ^{}}(𝐑,𝐤𝐪,t)`$ is the Hartree-Fock self-energy, with $`V_𝐪`$ standing for the Coulomb matrix element. In 2D case, $`V_𝐪`$ is given by $`V_𝐪=2\pi e^2/[ϵ_0(q+\kappa )]`$, with $`\kappa =(2e^2m^{}/ϵ_0)_\sigma f_\sigma (𝐤=0)`$ being the inverse screening length. $`ϵ_0`$ represents the static dielectric constant. It is noted that if one only takes account of the diagonal elements $`\rho _{\sigma \sigma }`$ and neglects all the off-diagonal elements $`\rho _{\sigma \sigma }`$ in Eq. (Spin oscillations in transient diffusion of a spin pulse in $`n`$-type semiconductor quantum wells), the first three terms on the left hand side of the equation correspond to the driving terms in the classical Boltzmann equation, modified with the DP term and the selfenergy term from the Coulomb Hartree contribution. $`\frac{\rho (𝐑,𝐤,t)}{t}|_c`$ and $`\frac{\rho (𝐑,𝐤,t)}{t}|_s`$ in the Bloch equations (Spin oscillations in transient diffusion of a spin pulse in $`n`$-type semiconductor quantum wells) are the coherent and scattering terms respectively. The coherent term describes the electron spin precession around the applied magnetic field and the effective magnetic field from the DP term. Its expression as well as that of the scattering term $`\frac{\rho (𝐑,𝐤,t)}{t}|_s`$ are given in detail in Refs. Weng and Wu, 2002 and Weng and Wu, 2003b.

It is noted that by using a spin-flip time $`\tau _{\text{sf}}`$ to describe the spin dephasing caused by the DP term and summing over the momentum, one is able to derive the diffusion equations for charge and spin densities of electrons in the so called “mean field” approximation.Ziese and Thornton (2001); Qi and Zhang (2003) However, as pointed out in our previous papers,Weng and Wu (2002) the adoption of the “mean field” approximation removes the interference between the electrons with different momentums and thus overlooks the inhomogeneous broadening that causes additional spin dephasing in the spin transport. We further point out in this paper that by using the spin-flip time approximation, some of the most marked features of the DP mechanism are thrown away.

We assume that at initial time $`t=0`$ there is a SPP centered at $`x=0`$. The electrons are locally in equilibrium, i.e., $`f_\sigma (x,𝐤,0)=\{\mathrm{exp}\left[(ϵ_k\mu _\sigma (x))/T_e\right]+1\}^1`$, where $`\mu _\sigma (x)`$ stands for the chemical potential of electrons with spin $`\sigma `$ at position $`x`$ and is determined by the corresponding electron density: $`N_\sigma (x,0)=_kf_\sigma (x,𝐤,0)`$. The shape of the initial spin pulse is assumed to be Gaussian like:

$$\mathrm{\Delta }N(x,0)=N_{\frac{1}{2}}(x,0)N_{\frac{1}{2}}(x,0)=\mathrm{\Delta }N_0e^{x^2/\delta x^2},$$
(2)
with $`\mathrm{\Delta }N_0`$ and $`\delta x`$ representing the peak and width of the SPP respectively. We further assume that there is no spin coherence at the initial time, $`\rho _{\sigma \sigma }(x,𝐤,0)=0`$. This SPP can be achieved by a circularly polarized laser pulse.

By numerically solving the kinetic equations (Spin oscillations in transient diffusion of a spin pulse in $`n`$-type semiconductor quantum wells) together with the initial conditions and the Poission equation (1), we are able to study the temporal evolution of the SPP with $`T=200`$ K and $`B0`$. A typical calculation of the spin diffusion in $`n`$-type GaAs QW is carried out by choosing the total electron density $`N_e(n_0(𝐑))=4\times 10^{11}`$ cm-2, the maximum spin imbalance in Eq. (2) $`\mathrm{\Delta }N_0=1\times 10^{11}`$ cm-2 and the width of the spin pulse $`\delta x=0.15\mu `$m. The material parameters are taken from Ref. Madelung et al., 1982. The absolute value of the spin imbalance $`|\mathrm{\Delta }N(x,t)|`$ and the incoherently summed spin coherenceWu and Ning (2000) $`\rho =_𝐤|\rho _{𝐤\sigma \sigma }(𝐑,t)|`$ are plotted as functions of the position $`x`$ along the diffusion direction and the time $`t`$ in Fig. 1 (a) and (b) respectively for impurity free case ($`N_i=0`$). Here $`N_i`$ denotes the impurity density. One can see from the figure that due to the strong diffusion as well as the spin dephasing, the spin polarization at the center of the spin pulse decays very fast initially. In the mean time, the spin coherence $`\rho `$ goes up due to the precession of spins in the presence of the effective magnetic field of the DP term. After 10 ps, as the diffusion becomes weaker due to the smaller spatial gradient, the decay rate at the center of the spin signal slows down and the spin coherence begins to decay due to the diffusion as well as the spin dephasing. It is noted that the spin polarization away from the center, e.g. in the region $`0.12`$ $`\mu `$$`<x<0.15\mu `$m, first increases due to the net spin diffusion from the center and then decays after the diffusion from the center becomes moderate. For the region out of the initial spin pulse ($`x>0.15`$ $`\mu `$m), the combined effect of the diffusion and the dephasing leads to more complicated behaviors. The most striking feature of the evolution of the SPP is that the spin polarization can be opposite to the initial one even in the absence of the applied magnetic field and there are oscillations in the time evolution of the spin polarization at some positions.

From Fig. 1(a) one can see that there is another peak in the spin polarization at the positions out of the initial spin pulse after 10 ps. However the spin polarization of this second peak is opposite to the initial one. As the time goes on, the second peak becomes larger due to the decay of the first peak in the center. After 30 ps, the heights of these two peaks are comparable. Moreover, in the region $`0.5\mu `$m$`<x<0.7\mu `$m, there are oscillations in the time evolution of spin polarization. The details are shown in Fig. 2 where the densities of the electrons with different spin $`N_\sigma (x,t)`$ are plotted at two typical positions $`x=0.54`$ and 0.65 $`\mu `$m for the cases with (dashed curves) and without (solid curves) impurities.

It is seen from Fig. 2(a) that at $`x=0.54`$ $`\mu `$m for impurity free case, there is no spin signal in the first picosecond as the position is located out of the initial spin pulse. Then the spin signal starts to build up due to the diffusion of both the diagonal electron distribution $`f_\sigma (x,𝐤,t)`$ and the off-diagonal spin coherence $`\rho _{𝐤\sigma \sigma }(x,t)`$ from the center. With the joint effects of the DP term as well as the diffusion, the spin signal reaches its first peak at about 2.5 ps and then decreases. It gets a crossing of spin-up and -down electron densities at 4 ps. After that the spin-down electrons exceed the spin-up ones and hence the spin polarization changes sign. The difference between the spin-up and -down electrons further increases until 7 ps when the difference arrives at another peak. The oscillations go on with the periods become larger and larger. After the third oscillation, the period becomes too long to observe any oscillation in the time regime of our calculation. As a result after the last crossing at 25 ps, the spin density of spin-down electrons is larger than that of the spin-up ones and the spin polarization is reversed. One can further see from the figure that, in the regime when the polarization oscillates, the spin coherence keeps increasing. This indicates that the spin coherence $`\rho `$ at this position mainly comes from the diffusion from the center. It is seen from the coherent terms of the Bloch equations that the imbalance of the distribution functions with the opposite spin and the spin coherence can transfer to each other by the DP effective magnetic field. Therefore, the additional spin coherence $`\rho `$ diffused from the center induces the spin polarization oscillations at position outside the initial spin pulse.

It is further noted that the oscillations differ in positions. For example, as shown in Fig. 2(b), at $`x=0.65`$ $`\mu `$m (and positions farther away), the oscillations are almost marginal but the feature that the spin polarization after a long time is opposite to the initial one remains. Moreover it is noted that in Fig. 2(a), when the spin pulse arrives, its polarization points to the initial one. Nevertheless, in Fig. 2(b) for positions farther away from the initial pulse, it is interesting to see that the spin signal arrives with spin polarization opposite to the initial one. This is understood that at positions far away from the initial pulse, what diffused from the center of the spin pulse is the off-diagonal spin coherence and the diagonal spin imbalance is quite small already at the edge of the initial pulse and therefore its diffusion to the outer space is marginal. The off-diagonal spin coherence induces the reverse of the spin polarization as what said above. This can be seen from the fact that for $`t<10`$ ps in Fig. 2(b), both diagonal and off-diagonal terms increase with time. For positions farther away from the center, the arrival of the spin polarization also includes the diagonal componants but with the opposite spin polarization.

We now explore the effect of the impurity to the spin diffusion. In Fig. 2 we also plot the corresponding curves of electron densities with impurity density $`N_i=0.1N_e`$ as dashed curves. The figure shows that the impurities dramatically change the behavior of the spin diffusion but do not eliminate the spin oscillations and the reverse of the spin polarization when time is long enough. By comparing the solid curves with the dashed ones it is noted that when time is long enough, say around 100 ps, the spin polarization for the case with impurities is always larger than that without impurities. This is understood that for the impurity free case, the mobility of electrons is larger and spin polarization is easier to diffuse away from the center. Moreover, the non-magnetic impurities tend to retain the spin coherence. This is because the impurity scattering drives the electrons to a homogeneous state in the momentum space and therefore counters the effect of the DP term that drives the electrons to an inhomogeneous state and leads to spin dephasing.Meier and Zakharchenya (1984); Wu and Ning (2000); Weng and Wu (2003b)

A similar spin oscillation without an applied magnetic field has been reported by Brand et al..Brand et al. (2002) Nevertheless it is noted that it is quite different from what discussed here. In the work of Brand et al., the spin oscillation happens in a spacial homogeneous system. And the oscillation is due to the breakdown of the assumption of the collision domination in the spin dephasing at extreme low temperature (a few Kelvin). For temperature higher than 10 K, the oscillation disappears as the electron collision rate increases and the assumption of the collision domination recovers. In our work, the spin oscillation comes from the diffusion (spacial gradient) and happens outside the initial spin pulse at very high temperature (200 K). The origin of the spin oscillation is therefore by no means only due to the small electron collision rates as in the case of Brand et al., but due to the combination of the diffusion and the precession of spin signals: At positions just outside of the initial spin pulse, the off-diagonal spin coherences of electrons with large momentums first reach there. As the DP term is proportional to the momentum, this fraction of electrons also share large precession frequencies. Therefore it is possible for the spin signal to oscillate at first few picoseconds and in the region just outside spin pulse when the collisions do not affect the momentum of electrons dramatically. As time passes by, the electrons with relatively smaller momentums, consequently with smaller precession frequencies, also arrive at the region where the oscillation occurs. Therefore due to the joint effects of the diffusion as well as the increasing impact of the collisions, the oscillation becomes slower and slower and totally vanishes after a few hundred picoseconds. For the spin signals in the center of the initial pulse there is no spin oscillation for the temperature of our investigation. This coincides with the results of Brand et. al.Brand et al. (2002) as well as what we discovered in high temperature cases.Weng and Wu (2003b)

The reverse and oscillation of the spin polarization of a spin pulse along the diffusion in the absence of the applied magnetic field can only be achieved when both the diagonal and off-diagonal terms of electron density matrix and the precession caused by the DP term are considered. Once the relaxation time approximation is adopted to describe the effect of the DP term or the off-diagonal term is dropped, the spin signal at the positions outside the initial SPP first increases due to the diffusion from the spin pulse then decreases monotonically due to the diffusion as well as the dephasing and the spin polarization never changes the sign. This is because in the framework of the relaxation time approximation, the most important difference between the spin dephasing caused by the DP mechanism and that caused by the other mechanisms is wiped off. Other spin dephasing mechanisms such as the Elliot-Yafet mechanismElliot (1954) and the Bir-Aronov-Pikus mechanism Bir et al. (1975) cause the spin dephasing through instantaneous spin-flip scattering. However, the DP term acts as a momentum dependent magnetic field around which the electron spins precess. This precession results in an inhomogeneous broadening in spin phases and leads to spin dephasing in the presence of the scattering. In additional to the dephasing, it is also possible that the precession may switch the magnetic momentum in the transport even without the applied magnetic field and in the high temperature regime. For some special positions, the combined effect of the diffusion and the precession may lead the spin to oscillate as shown in Fig. 2.

In conclusion, we perform a study of transient spin diffusion of a SPP in $`n`$-type GaAs QW’s by self-consistently solving the full kinetic Bloch equations in which both the diagonal terms, the distribution functions, and the off-diagonal terms, the inter-spin-band spin coherences, of the density matrix are included. We show that by taking the effect of the DP term to the diagonal and off-diagonal terms of the density matrix into account, the spin polarization outside the initial SPP can be reversed even without magnetic field. Moreover, for some special positions, the spin signals oscillate with time. The reverse and oscillations of the spin signals in spin diffusion/transport at positions outside the initial spin pulse have not been reported either theoretically or experimentally for $`n`$-type semiconductors and are understood from the diffusion of the off-diagonal terms of the electron density matrix which oscillates due to the precession of electron spins around the effective magnetic field due to the DP effect. We also stress that these features can only be achieved when the off-diagonal terms of the electron density matrix are included explicitly in the theory.

We would like to thank S. Zhang for his critical reading of this manuscript. MWW is supported by the “100 Person Project” of Chinese Academy of Sciences and Natural Science Foundation of China under Grant No. 90303012. MQW is partially supported by China Postdoctoral Science Foundation.


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# Influence of electromagnetic interferences on the gravimetric sensitivity of surface acoustic waveguides.

## 1 Introduction

Acoustic waves guided by the surface of solid structures form waveguides used as delay lines and filters in telecommunications . Waveguides support different modes with specific strain and stress fields . The acoustic velocity of each mode depends on different intrinsic and extrinsic parameters such as the mechanical properties of the materials, the temperature or the applied pressure. Waveguides are used as sensors when the velocity change is linked to environmental changes. For gravimetric sensors, the outer surface of the waveguide is exposed to mass changes. Due to the confinement of the acoustic wave energy close to the surface, these sensors are well suited for (bio)chemical sensors operating in gas or liquid environments. Among a wide variety of waveguides used for that purpose, Love mode sensors have attracted an increasing interest during the last decade . A Love mode is guided by a solid overlayer deposited on top of a substrate material. The usual substrates are piezoelectric materials like quartz, lithium tantalate and lithium niobate . Associated to specific crystal cut of these substrates, the Love mode presents a shear-horizontal polarization that makes it ideal for sensing in liquid media.

Current research in Love mode sensors concerns the guiding materials in order to obtain a high gravimetric sensitivity. Typical materials under investigations are dielectrics like silicon dioxide and polymers, and more recently semiconductors with piezoelectric properties like zinc oxide . Although the dispersion relation for Love mode is well set and the dependence of the gravimetric sensitivity of the liquid loaded sensor to the overlayer thickness has been thoroughly investigated , little has been devoted to study the role played by the structure of the sensor and the transducers.

In this paper, we investigate the role played by the structure of the sensor and the interferences between the acoustic and the electromagnetic waves on the gravimetric sensitivity. In the first part, we present a model of the transfer function including the influence of electromagnetic interferences. In the second part, we show how these interferences modify the gravimetric sensitivity in open and closed loop configurations of the sensor. Finally, these effects are illustrated experimentally on a Love mode sensor.

## 2 Modelling

Waveguide sensors consist of a transducing part and a sensing part. The transducing part includes the generation and the reception of acoustic signals and their interfacing to an electrical instrumentation. The most common transducers are the widespread interdigital transducers (IDTs) on piezoelectric substrates introduced by White and Voltmer in 1965 . Although the transducing part can be involved in the sensing part, practical sensing is confined to the spacing between the transducers. This confinement takes especially place when liquids are involved since these produce large and unwanted capacitive coupling between input and output electrical transducers. This coupling dramatically deteriorates the transfer function and is an important issue for the instrumentation of the sensors.

The sensor is a delay line formed by the transducers and the distance separating them. Each transducer is identified to its midpoint. The distance between the midpoints is $`L`$. The sensing part is located between the transducers and covers a total length $`D`$ so that $`DL`$. The guided mode propagates with a phase velocity $`V=\omega /k`$, where $`\omega =2\pi f`$ is the angular frequency and $`k=2\pi /\lambda `$ is the wavenumber. The waveguide is dispersive when the group velocity $`V_g=\omega /k`$ differs from the phase velocity.

The velocity is a function of the frequency and of the surface density $`\sigma =M/A`$ for a rigidly bound mass $`M`$ per surface area $`A`$. For an uniformly distributed mass, the surface density is rewritten in terms of material density $`\rho `$ and thickness $`d`$ by $`\sigma =\rho d`$. The phase velocity for an initial and constant mass $`\sigma _0`$ is denoted $`V_0`$, and the group velocity $`V_{g0}`$. In the sensing part, the phase velocity is $`V`$ and the group velocity $`V_g`$. According to this model, the transit time $`\tau `$ of this delay line is given by:

$$\tau =\frac{D}{V}+\frac{LD}{V_0}.$$
(1)
Electromagnetic interferences are due to the cross-talk between the IDTs. The electromagnetic wave (EM) emitted by the input transducer travels much faster than the acoustic wave and therefore is detected at the output transducer without noticeable delay. At the output transducer, the two kinds of waves interact with an amplitude ratio, denoted by $`\alpha `$, that creates interference patterns in the transfer function $`H(\omega )`$ of the delay line. The transfer function itself is given by the ratio of the output to the input voltages. The transfer function with electromagnetic interferences is modelled by the following equation:

$$H(\omega )=\underset{\mathrm{delay}\mathrm{line}}{\underset{}{H_0(\omega )\mathrm{exp}(\mathrm{i}\omega \tau )}}+\underset{\mathrm{EM}\mathrm{coupling}}{\underset{}{\alpha H_0(\omega )}}.$$
(2)
The transfer function $`H_0(\omega )`$ is associated to the design of the transducers. The total transfer function can be rewritten as $`H(\omega )=H(\omega )\mathrm{exp}\left(\mathrm{i}\varphi \right)`$ where expressions for the amplitude $`H(\omega )`$ and the phase $`\varphi `$ are obtained with help of complex algebra:

$`H(\omega )`$ $`=`$ $`H_0(\omega )\sqrt{1+2\alpha \mathrm{cos}(\omega \tau )+\alpha ^2};`$ (3)
$`\varphi `$ $`=`$ $`\varphi _0\mathrm{arctan}\left({\displaystyle \frac{\mathrm{sin}(\omega \tau )}{\alpha +\mathrm{cos}(\omega \tau )}}\right).`$ (4)
The phase $`\varphi _0`$ corresponds to the packaging of the sensor and is due to different aspects linked to the instrumentation. It will be assumed independent of the frequency and of the sensing event. The relations (3) and (4) are the sources of ripples in the transfer function at the ripple frequency $`\mathrm{\Delta }\omega =2\pi /\tau `$. The relative amplitude peak to peak of the perturbation on the amplitude has a maximum effect (in dB) equals to $`40\mathrm{log}[(1+\alpha )/(1\alpha )]`$. The amplitude (in dB and normalized to have $`H_0(\omega )=1`$) and the phase (in radians) as a function of the frequency are simulated in Figures 1 to 4 for different values of $`\alpha `$.

Under the influence of the interferences, the phase has different behaviors function of $`\alpha `$:

1. when $`\alpha =0`$ (no interferences), the phase is linear with the frequency and has a periodicity equal to $`2\pi `$ (Fig.1);
2. when $`\alpha <1`$, the phase is deformed but has still a periodicity equal to $`2\pi `$ (Fig. 2);
3. when $`\alpha =1`$, the phase has a periodicity equal to $`\pi `$ (Fig. 3);
4. when $`\alpha >1`$, the periodicity is lower than $`\pi `$ (Fig. 4);
5. when $`\alpha \mathrm{}`$, the phase is not periodic anymore and its value tends to $`\varphi _0`$.

This specific behavior of the phase has to be considered for the evaluation of the gravimetric sensitivity.

## 3 Gravimetric sensitivity

Changes in the boundary condition of the waveguide due to the sensing event modify phase and group velocities. As consequence, the transit time of the delay line and the phase of the transfer function are modified. The sensing event is quantified by recording the phase shift at a fixed frequency (open loop configuration) or the frequency shift at a fixed phase (closed loop configuration). This quantification gives rise to the concept of sensitivity. The sensitivity is the most important parameter in design, calibration and applications of acoustic waveguide sensors. Its measurement must be carefully addressed in order to extract the intrinsic properties of the sensor.

### 3.1 Sensitivity definitions

The gravimetric sensitivity $`S_V`$ is defined by the change of phase velocity as a function of the surface density change at a constant frequency. Its mathematical expression is given by Ref. :

$$S_V=\frac{1}{V}\frac{V}{\sigma }|_\omega .$$
(5)
The definition reflects the velocity change in the sensing area only while outside this area the velocity remains unmodified. The expression is general because the initial velocity $`V`$ of the sensing part does not need to be equal to $`V_0`$; this situation occurs in practical situations where the sensing part has a selective coating with its own mechanical properties, leading to a difference between $`V`$ and $`V_0`$.

To link the gravimetric sensitivity (caused by the unknown velocity shift) to the experimental values of phase and frequency shifts, we introduce two additional definitions related to the open and the close loop configurations, respectively. The phase sensitivity $`S_\varphi `$ is defined by

$$S_\varphi =\frac{1}{kD}\frac{\varphi }{\sigma },$$
(6)
and the frequency sensitivity $`S_\omega `$ is defined by

$$S_\omega =\frac{1}{\omega }\frac{\omega }{\sigma }.$$
(7)
### 3.2 Phase differentials without interferences

In order to point clearly the effects of the electromagnetic interferences on the different sensitivities presented in the previous section, we calculate the phase differentials in the ideal case of no interferences. For that case, the phase of the transfer function is a function of the frequency and the velocity, itself function of the frequency and the surface density:

$`\varphi (\omega ,V(\omega ,\sigma ))`$ $`=`$ $`\omega \tau `$ (8)
$`=`$ $`\omega \left({\displaystyle \frac{D}{V}}+{\displaystyle \frac{LD}{V_0}}\right).`$ (9)
Therefore, its total differential is:

$`\varphi `$ $`=`$ $`{\displaystyle \frac{\varphi }{\omega }}|_\sigma \omega +{\displaystyle \frac{\varphi }{\sigma }}|_\omega \sigma ;`$ (10)
$`=`$ $`\left({\displaystyle \frac{\varphi }{\omega }}|_V+{\displaystyle \frac{\varphi }{V}}|_\omega {\displaystyle \frac{V}{\omega }}|_\sigma \right)\omega +{\displaystyle \frac{\varphi }{V}}|_\omega {\displaystyle \frac{V}{\sigma }}|_\omega \sigma .`$ (11)
The derivative of the phase velocity as a function of the frequency comes from the definitions of phase and group velocities; at constant surface density we have from Ref. :

$$\frac{V}{\omega }|_\sigma =k^1\left(1\frac{V}{V_g}\right).$$
(12)
The other partial differentials are obtained by differentiation of Eq. (8):

$`{\displaystyle \frac{\varphi }{\omega }}|_V`$ $`=`$ $`\tau `$ (13)
$`{\displaystyle \frac{\varphi }{V}}|_\omega `$ $`=`$ $`{\displaystyle \frac{\omega D}{V^2}};`$ (14)
$`{\displaystyle \frac{\varphi }{\omega }}|_\sigma `$ $`=`$ $`\tau \omega {\displaystyle \frac{\tau }{\omega }}|_\sigma .`$ (15)
The partial differential of $`\tau `$ is given by

$$\frac{\tau }{\omega }|_\sigma =\left(\frac{D(V_gV)}{\omega VV_g}+\frac{(LD)(V_{g0}V_0)}{\omega V_0V_{g0}}\right)$$
(16)
and introduced in Eq. (15), it simplifies the expression in the form:

$$\frac{\varphi }{\omega }|_\sigma =\left(\frac{D}{V_g}+\frac{LD}{V_{g0}}\right).$$
(17)
In the case without dispersion, we have an equality between the partial derivative of the phase with respect to the frequency at constant surface density or at constant velocity as given by Eq. (1):

$$\frac{\varphi }{\omega }|_\sigma =\frac{\varphi }{\omega }|_V=\tau .$$
(18)
### 3.3 Open loop configuration

In the open loop configuration, the input transducer is excited at a given frequency while the phase difference between output and input transducers is recorded. This configuration with a constant frequency has $`\omega =0`$ in Eq. (11); related phase variations caused by surface density variations are obtained by

$`{\displaystyle \frac{\varphi }{\sigma }}`$ $`=`$ $`{\displaystyle \frac{\varphi }{V}}|_\omega {\displaystyle \frac{V}{\sigma }}|_\omega `$ (19)
$`=`$ $`{\displaystyle \frac{\varphi }{V}}|_\omega VS_V.`$ (20)
In the absence of interferences, phase variations obtained experimentally are directly linked to velocity changes by the product $`kD`$ involving the geometry of the sensor as seen by replacing Eq. (14) in Eq. (20):

$$\frac{\varphi }{\sigma }=kDS_V.$$
(21)
In other words: $`S_\varphi =S_V`$ when there are no interferences. In a first approximation $`k`$ is assumed equal to $`k_0`$ determined by the periodicity of the interdigitated electrodes in the transducer. This assumption is valid as long as the phase shift is evaluated close to the central frequency $`\omega _0=V_0k_0`$ and for waveguides with low dispersion. The wavelength is only known when the sensing part extends to the transducers ($`D=L`$). In that case, the transfer function of the transducers is modified as well by the velocity changes. In practice the value of the sensitivity is slightly underestimated to its exact value since $`kk_0`$, the error being of the order of $`5\%`$.

In the case where interferences occur, the partial differential of $`\varphi `$ with respect to the velocity is obtained by differentiation of Eq. (4):

$$\frac{\varphi }{V}|_\omega =\left(\frac{1+\alpha \mathrm{cos}(\omega \tau )}{1+2\alpha \mathrm{cos}(\omega \tau )+\alpha ^2}\right)\frac{\omega D}{V^2},$$
(22)
and the phase sensitivity is obtained by combining the latter equation with Eq. (20):

$$S_\varphi =\left(\frac{1+\alpha \mathrm{cos}(\omega \tau )}{1+2\alpha \mathrm{cos}(\omega \tau )+\alpha ^2}\right)S_V.$$
(23)
The influence of electromagnetic interferences on the phase sensitivity is simulated in Figure 5 versus the relative frequency for different values of $`\alpha `$. The phase sensitivity is always different compared to the gravimetric sensitivity. For the threshold value $`\alpha =1`$, the phase sensitivity is half of the gravimetric sensitivity; for higher values of $`\alpha `$, the phase sensitivity is always underestimated to the gravimetric sensitivity.

### 3.4 Closed loop configuration

In the closed loop configuration, the frequency is recorded while a feedback loop keeps the phase difference between output and input transducers constant. The configuration at constant phase has $`\varphi =0`$, the variation of the frequency as a function of the mass change is given by introducing this condition in Eq. (10):

$$\frac{\omega }{\sigma }=\left(\frac{\varphi }{\sigma }|_\omega \right)/\left(\frac{\varphi }{\omega }|_\sigma \right).$$
(24)
The upper term is replaced by Eq. (20). The phase slope as a function of the frequency at constant mass is obtained by differentiation of Eq. (4):

$$\frac{\varphi }{\omega }|_\sigma =\left(\frac{D}{V_g}+\frac{LD}{V_{g0}}\right)\left(\frac{1+\alpha \mathrm{cos}(\omega \tau )}{1+2\alpha \mathrm{cos}(\omega \tau )+\alpha ^2}\right).$$
(25)
We can establish a finalized equation taking into account the electromagnetic interferences by combining Eqs. (22) and (25) in Eq. (24):

$$S_\omega =\frac{D}{V}\left(\frac{D}{V_g}+\frac{LD}{V_{g0}}\right)^1S_V.$$
(26)
At the opposite of the open loop configuration, the frequency sensitivity is not influenced by the interferences. The perturbation caused by interferences on the aspect of the phase is cancelled by the closed loop configuration. However, as indicated by Eq. (26), the frequency sensitivity is strongly dependent of the structure of the sensor and the velocities in the different parts of the sensor. A simple expression can not be deduced easily and the link between the frequency sensitivity and the gravimetric sensitivity is difficult to exploit directly unless some assumptions are considered as explained here after.

If the waveguide is not dispersive and $`V=V_0`$, frequency variations obtained experimentally are directly linked to the gravimetric sensitivity by the ratio $`D/L`$ as seen by replacing the transit time obtained via Eq. (18) in Eq. (26):

$$S_\omega =\frac{D}{L}S_V.$$
(27)
If the waveguide is dispersive, the transit time $`\tau `$ contains the combined information of the group velocities in the transducing and sensing part and the phase velocity in the sensing part. If the sensing part extends to the entire delay line ($`D=L`$), we obtain an expression corresponding to a well-known result (for instance ):

$$S_\omega =\frac{V_g}{V}S_V.$$
(28)
## 4 Experimental results

For the practical consideration of the described behavior, we investigated a Love mode sensor. It was fabricated and tested under liquid conditions to evaluate the influence of the electromagnetic interferences. The Love mode was obtained by conversion of a surface skimming bulk wave (SSBW) launched in the direction perpendicular to the crystalline X axis of a $`500\mu \mathrm{m}`$ thick ST-cut ($`42.5^{}`$ Y-cut) quartz substrate. The conversion was achieved by a $`1.2\mu \mathrm{m}`$ thick overlayer of silicon dioxide deposited on the top side of the substrate by plasma enhanced chemical vapor deposition (Plasmalab 100 from Oxford Plasma Technology, England). Vias were etched in the silicon dioxide layer using a standard $`\mathrm{SF}_6/\mathrm{O}_2`$ plasma etch recipe. This process stopped automatically on the aluminium contact pads of the transducers.

The transducers consist of split fingers electrodes etched in $`200`$ nm thick sputtered aluminium. The fingers are $`5\mu \mathrm{m}`$ wide and equally spaced by $`5\mu \mathrm{m}`$. This defines a periodicity $`\lambda _0`$ of $`40\mu \mathrm{m}`$. The acoustic aperture defined by the overlap of the fingers is equal to $`80\lambda _0`$ (= 3.2 mm), the total length of each IDT is $`100\lambda _0`$ (= 4 mm) and the distance center to center of the IDTs is $`225\lambda _0`$ ($`L`$= 9 mm, $`D`$= 5 mm).

The sensing area was defined by covering the space left between the edges of the IDTs by successive evaporation and lift-off of 10 nm of titanium and 50 nm of gold in a first experiment, and 200 nm of gold in a second experiment. The fingers were protected against liquid by patterning photosensitive epoxy SU-8 2075 (Microchem Corp., MA) defining $`200\mu \mathrm{m}`$ thick and $`80\mu \mathrm{m}`$ wide walls around the IDTs. Quartz glasses of 5 by 5 $`\mathrm{mm}^2`$ were glued on top of the walls to finalize the protection of the IDTs.

The device was mounted and wire-bonded to an epoxy printed circuit board and its transfer function was recorded on a HP4396A Network Analyzer. This setup corresponds to the open loop configuration. Epoxy around the device covered and protected it and defined a leak-free liquid cell. The sensing area was immersed in a solution of $`\mathrm{KI}/\mathrm{I}_2`$ (4 g and 1 g respectively in 160 ml of water) that etched the gold away of the surface . The transfer function of the device was recorded every 4 seconds (limited by the GPIB transfer speed) during the etching of the gold with a resolution of 801 points over a span of 2 MHz centered around 123.5 MHz. The initial transfer function of the device is presented in Figure 6 with and without gold. The transfer function during etching of the 200 nm is shown at two moments (44 seconds and 356 seconds after etching start) in Figure 7. The total time for this etching was approximately 620 seconds. The sensitivity was calculated by etching of 50 nm of gold and assuming a density $`\rho =19.3\mathrm{g}/\mathrm{cm}^3`$. The result is plotted versus the frequency in Figure 8.

## 5 Discussion

Electromagnetic interferences have a clear effect on the transfer function because of the ripples they cause. The interaction modelled as a constant factor $`\alpha `$ is specific to each device and must be identified via a careful inspection of the transfer function. The amplitude of the transfer function peak to peak is supposed to be the product between the transfer function of the transducers and the interference, and therefore an evaluation of $`\alpha `$ is possible if the transfer function of the transducers only is known. However, the experiment shows that $`\alpha `$ is a function of the frequency and the surface density, indicating that finding its exact value is not straightforward. Only the phase indicates whether $`\alpha `$ is higher or lower than one.

In term of sensitivity, when $`\alpha 1`$ the phase has a periodicity $`P`$ in the range $`0`$ to $`\pi `$. We suggest the following correction to the experimental phase sensitivity:

$$S_\varphi =\frac{2\pi }{P}\frac{1}{kD}\frac{\varphi }{\sigma }.$$
(29)
This modification gives a better evaluation of the gravimetric sensitivity by stretching the phase of the transfer function to $`2\pi `$. Only the extraction of $`P`$ is not immediate since it depends upon $`\alpha `$.

Finally, we must mention that the experimental part is not exactly providing a differential surface density $`\sigma `$. Indeed, etching of $`50\mathrm{nm}`$ of gold corresponds to a surface density change of $`96.5\mu \mathrm{g}/\mathrm{cm}^2`$. This is a relatively large shift compared to the targeted biochemical recognition application where protein films surface density are in the order of $`500\mathrm{ng}/\mathrm{cm}^2`$. The evaluation of the sensitivity is best recorded by adding or etching thin layers of materials and that under the operating conditions of the sensor, especially if liquids are involved .

## 6 Conclusion

We have proposed a model for surface acoustic waveguides used as sensors. The model shows the influence of electromagnetic interferences caused by interdigital transducers on the gravimetric sensitivity in open and closed loop configurations. In both cases, the dimensions of the delay line and the sensing part influence the experimental value of phase or frequency shifts.

In an open loop configuration and with interferences, the phase shift is disturbed and the sensitivity is over- or under-estimated to the value of the gravimetric sensitivity. For strong interferences, the phase has a periodicity lower than $`2\pi `$ that must be considered when normalizing the phase shift to obtain a correct figure of the sensitivity.

In a closed loop configuration and with interferences, the frequency shift is not disturbed. The frequency shift is proportional to the sensitivity by the ratio between the length of the sensing area and the distance separating the transducers. In addition, the frequency shift is influenced by the dispersive properties of the waveguide.

The influence of the electromagnetic interferences on the transfer function of a Love mode sensor operating in liquid conditions was presented for a comparison. From the experiment it appears that the interferences are function of both the frequency and the surface density.

For future investigations, an analytical expression of the electromagnetic-acoustic interaction and the parameters acting on it have to be identified in order to reduce the influence or, on the opposite, to enhance the gravimetric sensitivity of surface acoustic waveguides.

## 7 Acknowledgements

L. Francis is thankful to N. Posthuma for the support with the PECVD tool, to C. Bartic for the SU8 walls fabrication, and to the belgian F.R.I.A. fund for financial support.

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Figure 5

Figure 6

Figure 7

Figure 8


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# Exposing the spin glass ground state of the non-superconducting La2-xSrxCu1-yZnyO4 high-𝑇_𝑐 oxide

## Abstract

We have studied the spin glass behaviour of non-superconducting La2-xSrxCu0.95Zn0.05O4 ($`x=0.100.22`$). As in the superconducting analogues of these samples the spin glass transition temperature $`T_g`$ decreases with increasing $`x`$, and vanishes at $`x=0.19`$. A local enhancement in $`T_g`$ at $`x=0.12`$ is also observed and attributed to stripe ordering. The disappearance of $`T_g`$ for $`x0.19`$ is discussed in terms of a quantum phase transition.

The prototype oxide La2CuO4 is an example of a diluted quantum antiferromagnet in which the Neel temperature decreases with doping and added holes are believed to segregate, at first, into stripes Sachdev ; Kivelson ; Zaanen ; Smith . La2CuO4 undergoes an insulator-superfluid transition by hole doping, and this is generally explored by replacing La3+ with Sr2+ to form La2-xSrxCuO4. Early works indicated that for $`x>0.01`$ La2-xSrxCuO4 changes from a long-range antiferromagnetic insulator to a spin glass, characterised by a cusp in magnetisation at the glass transition temperature $`T_g`$ and an associated field hysteresis below Chou ; Wakimoto ; Lavrov ; Kastner . The critical exponents and memory effect were found to be in good agreement with conventional spin glass systems, although a crystallographic directional dependence, possibly related to the presence of stripes, was observed. Nevertheless, the onset of spin glass behaviour in all three principle crystallographic directions was shown to be associated with an order parameter and broken symmetry due to frozen spins SFE1 ; SFE2 .

Similar magnetisation studies cannot be performed for $`x>0.05`$ due to masking of the thermodynamic spin glass characteristics by the onset of superconducting diamagnetism. However, other reliable methods such as neutron scattering, nuclear magnetic resonance and muon spin relaxation ($`\mu `$SR) have been successfully employed to investigate spin glass behaviour across the ($`T,x`$) phase diagram of HTS Wakimoto ; Kastner ; Wakimoto2 ; Matsuda ; Budnick ; Harshman ; Kiefl ; Sternlieb ; Niedermayer ; Singer1 ; Singer2 ; Hunt ; Julien1 ; Julien2 ; Julien3 ; CP1 ; CP2 ; CP3 . Although $`T_g`$ obtained from spectroscopic techniques may vary depending on their frequency window there is good agreement with thermodynamic measurements where available. Over the past several years various spectroscopic studies have shown $`T_g`$ to extend into the superconducting dome of the HTS phase diagram indicating coexistence of superconducting and spin glass order. Furthermore, a comprehensive $`\mu `$SR study in several HTS showed that $`T_g`$ ceases to exist at a critical doping $`x_c`$ $``$0.20 suggesting the presence of a quantum glass transition CP1 ; CP2 ; CP3 .

However, it remains to be confirmed that $`x_c`$ is in fact robust with respect to the energy window of $`\mu `$SR. That is, if the absence of dynamical relaxation for $`x>x_c`$ is independent of the energy scale of the spin fluctuations, hence the presence of an unambiguous quantum transition. To address this question we have exposed the normal state magnetic ground state of La2-xSrxCuO4 across the superconducting dome. Instead of using an applied field, which is beyond experimental capabilities, we use non-magnetic Zn, to suppress superconductivity. Substituting zinc for copper also slows down the spin fluctuations, suppresses long range order, and on the basis of systematic $`\mu `$SR studies it enhances the muon depolarisation rate at low temperatures and increases $`T_g`$ CP2 ; Kimura . These effects allow us to eliminate possible masking of a short-range magnetic order due to the $`\mu `$SR frequency limit. A disadvantage in using zinc is that the exposed ground state is distorted and therefore not pristine. However, this does not affect the aim of the present work since we are mainly interested in the evolution of short-range magnetic order.

The materials studied were La2-xSrxCu0.95Zn0.05O4 ($`x`$=0.10-0.22). Samples were synthesised using solid-state reaction and where necessary followed by quenching and subsequent oxygenation. Spectroscopic, chemical and elemental analyses showed them to be phase pure and stoichiometric. Magnetisation measurements indicated $`T_c`$=0 in all samples. Zero-field (ZF) and longitudinal-field (LF) $`\mu `$SR studies were performed at the pulsed muon source, ISIS Facility, Rutherford Appleton Laboratory. In a $`\mu `$SR experiment, $`100\%`$ spin-polarised positive muons implanted into a specimen precess in their local magnetic environment. Random spin fluctuations will depolarise the muons provided they do not fluctuate much faster than the muon precession. The muon decays with a life-time $`2.2\mu s`$, emitting a positron preferentially in the direction of the muon spin at the time of decay. By accumulating time histograms of such positrons one may deduce the muon depolarisation rate as a function of time after implantation. The muon is expected to reside at the most electronegative site of the lattice. As discussed previously in La2-xSrxCu1-yZnyO4 it is the apical O2- nearest to the planes so the results reported here are dominated by the magnetic correlations within the CuO2 planes CP2 ; Nachumi .

Figure 1 (left-hand-side panels) shows the time dependence of the ZF muon asymmetry for La2-xSrxCu0.95Zn0.05O4 with $`x`$=0.10 - 0.18. All samples exhibit glassy behaviour with $`x=0.18`$ (at $`T=0.03`$K) being just at the threshold of glassiness. A characteristic signature of a spin-glass within a $`\mu `$SR spectrum is a rapid initial relaxation followed by a much slower and more gradual long-term relaxation Uemura . This can be explained by considering the muon lifetime within the glass: upon insertion, the spin-polarised muons are greeted by a distribution of randomly aligned magnetic fields. Since these fields are quasi-static the detected asymmetry relaxes very quickly. The ensuing longer-term relaxation is due to a small number of low-frequency fluctuations, which may still be present in the CuO2 planes of the samples. Let us note that in a typical spin glass system a single pronounced dip is expected after the sharp drop in asymmetry Uemura . However, this behaviour is not universal among systems exhibiting short range ordered magnetism, including HTS, and should not be viewed as the essential condition for characterising spin glass behaviour Budnick ; Harshman ; Kiefl ; Sternlieb ; Niedermayer ; CP1 ; CP2 ; CP3 ; Uemura ; BDR . Furthermore, as discussed above, other studies in HTS such as neutron scattering and nuclear magnetic resonance, also show clear evidence for spin glass behaviour. Most importantly however, it is in the temperature region where the ZF $`\mu `$SR spectrum shows the rapid initial relaxation that thermodynamic measurements exhibit a well-defined field-dependent magnetic transition and associated thermal hysteresis at $`T_g`$, indicating glassy short-range magnetic ordering with an associated order parameter Chou ; Wakimoto ; Lavrov ; Kastner . The right-hand-side panels of Fig. 1 depict typical spectra obtained with an external longitudinal field applied parallel to the initial muon spin polarisation. The field dependence of the spectra indicates that the spins depolarising the muons are static and as the applied field increases the depolarisation decreases and the asymmetry eventually recovers its initial value.

The $`x`$=0.18 sample displays a much slower relaxation compared with $`x<0.18`$ but still clearly indicates the presence of a glass at the lowest temperature ($`T`$=0.03K). It shows three characteristic indications that it has already entered the glassy phase. Firstly, the spectrum relaxes much quicker than the heavily over-doped samples; secondly, it follows the field dependence of samples $`x`$=0.10 - 0.16 and thirdly, the rate of change of the gradient in the asymmetry spectrum ($`i.e.`$ the second derivative) is positive rather than negative. The spectra for $`x0.19`$ were Gaussian at all temperatures (see e.g. Fig. 2(a)).

The inset for the ZF-plot for $`x=0.10`$ in Fig. 1 shows ZF-data for $`x`$=0.10 and 0.12 at short-times. We find that at very small time scales $`x=0.10`$ and $`x=0.12`$ (multiplied by 1.3 for clarity) exhibit a faint oscillation which quickly fades as time increases. These oscillations are enhanced at lower temperatures and doping and are successfully fitted by including a precessing component in the Kubo-Toyabe function Niedermayer ; Akoshima ; Savici ; Adachi . Oscillations are only observed for $`x<0.13`$ and $`y=00.05`$ and can only be due to the precession of the muon spins around a stronger non-random internal field caused by the presence of an ordered magnetic state. For example, an antiferromagnetic ground state may be present here. This has also been inferred from neutron scattering experiments for $`x`$=0.11 Lake . We speculate that these oscillations may be related to the presence of stripes Niedermayer ; Akoshima ; Savici ; Adachi . At this doping range most HTS show a small drop or a plateau in $`T_c`$ and in the superfluid density CP1 ; CP2 ; Kivelson2 . The exact reason for this drop is unclear, but it is thought that there is an enhanced tendency towards magnetic ordering at this point due to some peculiarity in the structural orientation of the CuO6 octahedra. This has the effect of creating strongly correlated antiferromagnetic stripe domains. It is these stripes which may provide the spin correlations causing the muon precession. This stripe arrangement is reminiscent of the antiferromagnetic phase present for $`x<0.02`$ and raises the question as to whether there is a hidden weak antiferromagnetic ground state present in other regions of the phase diagram of La2-xSrxCuO4. Further investigations on this matter are to be carried out.

As the temperature is increased, samples displaying glassy behaviour exhibit a gradual change in the spectra. A typical example, $`x=0.10`$, is shown in Fig. 2(c). In glassy samples ($`x<0.19`$), at high temperature the depolarisation is Gaussian and temperature independent, just like $`x0.19`$, consistent with dipolar interactions between the muons and their near-neighbour nuclear moments. This was verified by applying a small longitudinal magnetic field (30G) to the $`x`$=0.14 sample at 50K in order to ascertain the origin of the muon response (Fig. 2(d)). The field due to the nuclear moments is extremely weak (much weaker than the internal field present for a spin-glass). Therefore, nuclear decoupling leading to a collapse in the response function should result following application of even a very low field as shown in Fig. 2(d). The Gaussian behaviour at high temperature was verified also for the samples with lower hole-dopings. Furthermore, a 30G field was also applied to the $`x`$=0.19 sample at $`T`$=0.03K and 0.75K to check for nuclear decoupling (Fig. 2(b)). The muon response was again observed to collapse, for the same field at both temperatures, showing that there is no evidence for low-energy electron spin fluctuations or onset of glassy behaviour for $`x0.19`$.

As in earlier works CP1 ; CP2 ; CP3 , two characteristic temperatures for use in the analysis of the slowing of the spin fluctuations have been determined. These are the temperature $`T_f`$ where the spin correlations first enter the $`\mu `$SR time window, $`i.e.`$ where the muon asymmetry first deviates from Gaussian behaviour and the temperature $`T_g`$ at which these correlations freeze into a glassy state thus causing an initial rapid decay in the asymmetry. The evolution of the muon spin with time ($`i.e.`$ its relaxation) may be fitted to the form $`G_z(t)=A_1exp(\lambda _1t)+A_2exp((\lambda _2t)^\beta )+A_3`$ where the first term is the fast relaxation in the glassy state ($`i.e.`$ $`A_1`$=0 for $`T>T_g`$), the second stretched-exponential term describes the slower relaxation of the dynamical spins and $`A_3`$ accounts for a small time-independent background arising from muons stopping in the silver backing plate of the sample holder. As in some other spin glass systems, $`\beta `$ is constant (with the value $`\beta `$=2) in the high-temperature Gaussian limit (Fig. 3) Uemura ; BDR . The temperature where $`\beta `$ starts decreasing (Fig. 3) and the spin lattice relaxation rate $`\lambda `$ increasing ($`e.g.`$ Fig. 3 (inset to $`x`$=0.10)) is regarded as the onset temperature, $`T_f`$, at which spin fluctuations slow down sufficiently to enter the frequency scale of the muon probe ($`10^{10}`$s).

Now, to address the question of a possible quantum phase transition at $`x_c`$, we concentrate on the freezing temperature, $`T_g`$, for which thermodynamic measurements indicate an associated spin glass order parameter. In ZF-$`\mu `$SR $`T_g`$ is identified as the temperature where $`\beta `$ falls to 0.5$`\pm 0.06`$ BDR . This root exponential form for the relaxation function is a common feature of spin glasses. It should be noted that different fitting procedures for estimating $`T_g`$ consistently yield similar values CP2 ; Kanigel ; Keren . It is also at $`\beta `$=0.5 where the spin lattice relaxation rate, as obtained from the same fits, reaches a maximum, as shown in the inset to Fig. 3 for $`x`$=0.10. This confirms $`\mu `$SR as a credible technique to accurately identify and characterise spin-glass behaviour. Figure 3 shows the variation of $`\beta `$ with temperature for some of the samples studied. At first glance we see the onset (where $`\beta `$ starts falling) and freezing of spin fluctuations vary in the same manner as found for pure, 1 and 2 $`\%`$ Zn doped La2-xSrxCuO4, $`i.e.`$, decreasing with increasing doping. Furthermore, for $`x0.19`$, there are no changes in the depolarisation function and $`\beta `$ is almost temperature independent, consistent with Gaussian depolarisation. It is clear from the data that changes in the magnetic ground state occur at $`x=0.19`$. The main contribution of the present study is that superconductivity has been fully suppressed and therefore any masked or hidden magnetism is now exposed. This was important to demonstrate experimentally since earlier works left question marks as to whether changes in the measured magnetic ground state were reflecting actual changes in ground state of the material, or were an artefact of the presence of superconductivity.

Values of $`T_g`$ summarised in Fig. 4 indicate a gradual decrease of the onset of the spin glass phase with doping. The exception is the $`x=0.12`$ sample for which $`T_g`$ is higher than for $`x=0.10`$. We note the positive curvature of $`T_g(x)`$, exactly as seen previously for pure, 1 and 2 $`\%`$ Zn doped La2-xSrxCuO4 and pure Bi2.1Sr1.9Ca1-xYxCu2O8+y, and expected in quasi-2D systems like the HTS CP1 ; CP2 ; CP3 . The increase in $`T_g`$ in the 1/8 region has been previously discussed in terms of stripe domains CP1 ; CP2 ; CP3 ; Akoshima ; Adachi . The effect of the ordered phase is also evident for $`x=0.14`$, which from the trend of $`T_g(x)`$ indicates the latter is higher than expected for this doping. In fact the presence of a static stripe component for $`x=0.14`$ can be seen in neutron scattering experiments Kivelson2 ; Hirota . Here the order parameter is small and is unlikely to be homogeneous which is consistent with the absence of a well-defined precession frequency in our $`\mu `$SR measurements. The spin glass regime vanishes at $`x=0.19`$ and for $`x0.19`$ we did not observe even an onset ($`T_f`$) of spin fluctuations slowing down sufficiently to enter the frequency scale of the muon probe (Fig. 4). The field dependent studies (see e.g. Fig. 1) enabled us estimate the internal local field, $`B_{local}`$, sensed by the implanted muons Satooka . Fig. 4 also includes the doping dependence near $`x_c`$ of $`B_{local}`$, measured at $`T=0.03`$K. This exhibits a behavior similar to $`T_g`$ and $`T_f`$ and disappears at precisely $`x=0.19`$.

The observation $`T_{g,f}(x)`$=0 and $`B_{local}`$=0, at $`x0.19`$ $`for`$ $`all`$ $`Zn`$ $`concentrations`$ indicates that spin glass and low frequency fluctuations disappear at $`x_c`$ and earlier results to this effect were not masked by either the frequency window of the technique or the presence of superconductivity. Similar conclusions have been reached by recent Cu-nuclear quadropole resonance studies Yamagata . Bearing in mind the fact that $`T_f`$ and $`T_g0`$ at $`x=0.19`$ so that the rate of slowing down actually diverges at this point, the present results support the existence of a quantum glass transition at $`x_c`$. Assuming, based on extrapolation from magnetisation studies for $`x<0.05`$ Chou ; Wakimoto ; Lavrov ; Kastner  and the systematic trends of the $`\mu `$SR spectra across the many different samples we have so-far investigated, the quantum glass transition is a conventional spin glass transition, in the sense that it has an associated order parameter and symmetry breaking at $`T=0`$, then we may interpret the glass transition at $`T=0`$ as a quantum critical point.

We note that the values for $`T_g(x)`$ for $`y=0.05`$ are lower than those found in earlier studies for $`y=0.02`$ even though $`T_g(x)`$ was found to increase systematically for $`x=`$0, 0.01 and 0.02 CP2 ; CP3 . This presumably occurs because, while Zn slows the spin fluctuations, it also dilutes the spins and at high concentration we see the latter effect. Nevertheless, zinc substitution has undoubtedly exposed the ground state, however distorted it might be, in the samples studied here and allowed us to identify the precise location ($`x=0.19`$) at which the spin glass disappears. Based also on the systematic tendency of $`T_g`$ and $`T_f`$ to vanish at $`x=0.19`$ it is unlikely $`y=0.05`$ has suppressed short-range magnetic order only for $`x0.19`$. Therefore, we can safely confirm our earlier indications that the magnetic ground state of HTS changes character at $`x_c`$, independent of the presence or absence of superconductivity.

Other properties also show distinct changes near $`x_c`$. Recent resistivity studies in $`both`$ pure and Zn doped high-$`T_c`$ oxides showed the transition from a pseudogap towards a Fermi liquid phenomenology Naqib . Evidence for a change in the ground state has been reported CP4  for the most fundamental measurable quantity in superconductivity, namely the superfluid density $`\rho ^s`$. Both the $`ab`$-plane and $`c`$-axis superfluid response in La2-xSrxCuO4 and HgBa2CuO4+δ were found to remain relatively constant above $`x_c`$ but drop rapidly below $`x_c`$. Furthermore, at 0.19 holes per planar copper atom there is a peak in $`\rho ^s(0)`$ for HgBa2CuO4+δ indicating the strongest superconductivity at the point where $`T_g`$ vanishes. Also, the doping dependence of the anisotropy in the penetration depth indicates a crossover from two- to three-dimensional transport. These changes in the superconducting ground state, taken together with the disappearance of the spin glass order at the same doping at $`T=0`$, point consistently to a simultaneous change in the ground state symmetry and superconductivity, as expected in a quantum critical point scenario.

In summary, we have suppressed $`T_c`$ across the superconducting dome of the La-cuprate family. These samples allowed us to take earlier studies a step further and provide new experimental evidence for absence of short-range magnetism for $`x0.19`$. The experiments support the presence of a quantum glass transition at $`x=0.19`$, as also reflected in the disappearance of spin-glass order and the change in the superconducting ground state.

Acknowledgements: We thank ISIS for the continuing support of this project. C.P. thanks S. Chakravarty and S. Sachdev for useful discussions, and The Royal Society for a University Fellowship. JLT acknowledges financial support from the Marsden Fund.

FIGURE CAPTIONS

FIG. 1. The panels on the left-hand-side show zero-field $`\mu `$SR spectra for La2-xSrxCu0.95Zn0.05O4 for $`x`$=0.10 - 0.18. The solid lines are the fits discussed in the text. The right hand panels show the suppression of the glass transition in presence of longitudinal fields. The solid lines are drawn as guide to the eye. The inset shows oscillations seen for $`x`$=0.10 and 0.12 at low times. The $`x=0.12`$ data have been shifted for clarity. Data were taken at the temperatures indicated in the respective panels.

FIG.2. (a) Zero-field $`\mu `$SR spectra for La2-xSrxCu0.95Zn0.05O4 ($`x=0.19`$)at different temperatures as indicated in the figure. (b) Suppression of the asymmetry of $`x=0.19`$ at $`H`$=30G at two different temperatures (see text for details). (c) Zero-field $`\mu `$SR spectra for $`x`$=0.10 measured at different temperatures: $`T`$=1.3K (crosses), 5K (squares), 7K (closed circles), 15K (open circles) and 50K (triangles). (d) Muon asymmetry for $`x`$=0.14 at high temperature being suppressed by a 30G applied longitudinal field.

FIG. 3. Typical temperature dependence of the (stretched-exponential) exponent $`\beta `$ obtained by fitting muon depolarisation data for La2-xSrxCu0.95Zn0.05O4 ($`x`$=0.10, 0.14, 0.16, 0.18, 0.19 and 0.22). The inset to $`x`$=0.10 shows the temperature dependence of the spin lattice relaxation rate for the same sample.

FIG. 4. The doping dependence of the temperature $`T_g`$, below which the spin fluctuations freeze out into a spin glass, for La2-xSrxCu0.95Zn0.05O4 ($`x`$=0.10-0.22). Also shown are data for $`T_f`$ and $`B_{local}`$ near $`x_c`$.