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# Huge enhancement of electromechanical responses in compositionally modulated Pb(Zr1-xTix)O3

Monte Carlo simulations based on a first-principles-derived Hamiltonian are conducted to study the properties of Pb(Zr1-xTix)O3 (PZT) alloys compositionally modulated along the  pseudocubic direction near the morphotropic phase boundary (MPB). It is shown that compositional modulation causes the polarization to continuously rotate away from the modulation direction, resulting in the unexpected triclinic and C-type monoclinic ground states and huge enhancement of electromechanical responses (the peak of piezoelectric coefficient is as high as 30000 pC/N). The orientation dependence of dipole-dipole interaction in modulated structure is revealed as the microscopic mechanism to be responsible for these anomalies.

Complex perovskite alloys have been studied for more than fifty years, which are of great importance not only because they have wildly technical applications for their large electromechanical responses,KU  but also because they are fundamentally interesting for their anomalous properties and the relations to the microscopic structure. Recently, two breakthroughs were achieved in the research of complex perovskites. One is the observation of large enhancement of piezoelectric constants in single crystals.Park ; Serv  The second is the discovery of a low-temperature monoclinic phase in Pb(Zr1-xTix)O3 (PZT) near the morphotropic phase boundary (MPB).BN1 ; BN1a  Inspired by such progresses, lots of works were done to search larger electromechanical response and unobserved phases in complex perovskites. Particularly, an ab initio calculation on Pb(Sc0.5Nb0.5)O3 (PSN) revealed that atomic rearrangement would lead simultaneously to large electromechanical responses and unusual structural phases.AM  The difference between the valences of the B atoms (Sc3+ and Nb5+) was pointed out to be the main reason for the existence of these anomalous properties and this mechanism is expected to be generally applicable in a given class of heterovalent perovskite alloys, which is likely to have large technological and fundamental implications. However, it is unclear whether there is any interesting effect in the modulated homovalent systems where the B atoms have the same valences.

In this letter, we investigate the influences of compositional modulation on the homovalent PZT solid solutions near MPB. Remarkably, it is found that the atomic ordering along the  direction leads to the suppression of $`P_x`$ ($`x`$-component of the polarization). Unexpected new ground states of triclinic (Tri) and C-type monoclinic (MC) phases appear with greatly enhanced piezoelectric coefficients. The orientation dependence of dipole-dipole interaction in modulated structure is revealed to be responsible for these anomalies. Such microscopic mechanism is expected to work in MPB region of any homovalent perovskite when the atomic ordering is produced.

We adopt the effective Hamiltonian of PZT alloys proposed by Bellaiche, Garcia and Vanderbilt, LB1  which is derived from first-principles calculation, to predict the properties of compositionally modulated PZT structures by conducting Monte Carlo simulations. In this scheme, the total energy $`E`$ is written as the sum of an average energy and a local energy asLB1 ; LB2

$`E(\{𝐮_i\},\{𝐯_i\},\eta _H,\{\sigma _j\})`$ $`=`$ $`E_{\mathrm{ave}}(\{𝐮_i\},\{𝐯_i\},\eta _H)`$ (1)
$`+E_{\mathrm{loc}}(\{𝐮_i\},\{𝐯_i\},\{\sigma _j\}),`$
where $`𝐮_i`$ is the local soft mode in unit cell $`i`$, $`𝐯_i`$ is the dimensionless local displacement related to the inhomogeneous strainWZ , $`\eta _H`$ is the homogeneous strain tensors and $`\sigma _j=\pm 1`$ represents the presence of a Zr or Ti atom, respectively, at lattice site $`j`$ of the PZT alloy. All the parameters of Eq. (1) are derived from the first principle calculations and are listed in references.LB1 ; LB2  The modulated structures under consideration are made of the sequences Pb(Zr1-x+νTix-ν)O3/Pb(Zr1-x-νTix+ν)O3 along the  direction with B atoms randomly distributing within each  plane. 10$`\times `$10$`\times `$10 or 12$`\times `$12$`\times `$12 supercells with periodic boundary conditions are used in Monte Carlo simulations to get well converged results. Eq. (1) is based on the virtual crystal approximation (VCA).No ; LB4  The parameters of Zr and Ti atoms are composition-dependent, which reflects an average influence from surrounding atoms. Considering that the modulation length of our studied structures is small (only two monolayers) and a Zr or Ti atom will be influenced by atoms from planes with different compositions, we adopt the parameters corresponding to the overall composition $`x`$ for all atoms in the modulated structures. Some detailed tests are also carried out, which show that the anomalous properties of the modulated structures revealed in this paper are not sensitive to the choice of parameters.

First we consider the properties of modulated PZT as a function of composition $`x`$ by setting parameter $`\nu `$ to its maximum value ($`\nu =x`$). Fig. 1(a) shows the cartesian coordinates ($`u_x,u_y,u_z`$) of the supercell average of the local mode vectors at $`T`$=50K. (Due to the difference between the theoretical and experimental temperatures,LB1  it corresponds to an “experimental” temperature around 30K.) In the non-modulated case, it was demonstrated that disordered Pb(Zr1-xTix)O3 has a pseudocubic  direction polarized ($`u_x=u_y=u_z>0`$) rhombohedral phase (R) for $`x<0.475`$, a  direction polarized ($`u_x=u_y=0<u_z`$) tetragonal phase (T) for $`x>0.49`$, and a A-type monoclinic phase (MA) with $`0<u_x=u_y<u_z`$ for $`0.475<x<0.49`$.LB1 ; LB2  In the modulated case, for compositions outside MPB, the local mode vectors are slightly affected as shown in Fig. 1(a). However, the precise symmetry has been changed by the atomic ordering, and the phases are recognized as B-type monoclinic (MB) and orthorhombic (O). The interesting phenomena appear within the MPB region. For $`0.480<x<0.485`$, $`u_x`$ decreases drastically, which results in a triclinic (Tri) phase with $`u_xu_yu_z`$. When $`x`$ is larger than 48.5%, $`u_x`$ vanishes and an unexpected ground state appears in the modulated systems: a C-type monoclinic (MC) phase with $`0=u_x<u_y<u_z`$. Fig. 1(a) thus depicts a polarization rotation in modulated PZT structures following the sequence of MB-Tri-MC-O as the Ti composition increases. Although Tri and MC phases in PZT were first demonstrated in the simulation of electric-field induced transformation in disordered rhombohedral PZT by Bellaiche et al.,LB3  it has not been observed experimentally yet because the predicted electric field required to induce the Tri and MC phases is too high ($``$ 500 kV/cm for composition close to MPB) compared with what experiments can provide. Thus the present study demonstrates an alternative routine to observe such phases with less experimental obstacles.

Fig. 1(b) shows the corresponding piezoelectric coefficients and Fig. 1(c) the dielectric susceptibilities which are calculated in the correlation-function approachAG . It shows that $`d_{15}`$ reaches its maximum near the Tri to MC transition and remains a remarkably large value above 1000 pC/N in MPB region, while $`d_{24}`$ achieves values above 1000pC/N in MC phase and reaches its maximum near the MC to O transition. Another important piezoelectric coefficient, $`d_{33}`$, is not shown here because the modulations scarcely affect $`u_z`$ and have little effect on $`d_{33}`$. The existences of the MB-Tri, Tri-MC and MC-O transitions also result in the peaks of dielectric responses, as shown in Fig. 1(c).

We also investigate the effects of the modulation parameter $`\nu `$, the fluctuation amplitude, on the structural and piezoelectric properties of the modulated structures which have overall composition $`x=0.485`$. Fig. 2(a) shows the average local modes as a function of $`\nu `$ at 50K. The structure of $`\nu =0`$ (in the case of disordered PZT alloy) has $`u_x=u_y<u_z`$ characterizing the MA structure with polarization lying between  and  directions. When $`\nu `$ becomes larger than 0.155, $`u_x`$ begins to decrease. With increasing $`\nu `$, $`u_x`$ decreases gradually whereas $`u_y`$ and $`u_z`$ increase very slowly. This behavior corresponds to the phase with a Tri symmetry. When $`\nu `$ becomes larger than 0.45, $`u_x`$ becomes null, while $`u_y`$ and $`u_z`$ remain unequal, indicating a MC symmetry with a polarization between  and  directions. Summarily, increasing the parameter $`\nu `$ leads to a continuous rotation of the polarization and transformation between different ground states which are driven by the annihilation of $`u_x`$—the polarization component along the direction of compositional modulation.

Theoretical and experimental studies have suggested that polarization rotation is essential for the large piezoelectric response in the perovskite alloys.HF ; BN3  Such an effect is clearly demonstrated in Fig. 2(b) where the piezoelectric coefficient $`d_{15}`$ is depicted. With decreasing $`u_x`$, $`d_{15}`$ increases from 2000 pC/N to 8000 pC/N gradually in the Tri phase for $`0.2<\nu <0.4`$. Then $`d_{15}`$ reaches a very steep peak about 30000 pC/N at $`\nu 0.4`$ where the polarization most easily rotates \[see also Fig. 2(a)\]. After that, $`d_{15}`$ decreases slowly but still remains large values even in Mc phase. As one can see in Fig. 2(b), $`d_{15}`$ is larger than 10000 pC/N for a broad range of $`\nu >0.4`$. To our best knowledge, such a huge enhancement of the piezoelectric coefficient has never been reported in any perovskite material before.

Temperature properties of the material are important for its application performances. Here we investigate the influence of temperature on a structure with $`x=0.485`$ and $`\nu =0.305`$, which adopts a Tri ground state in Fig. 2(a). The resulting piezoelectric properties are depicted in Fig. 3. A huge $`d_{24}`$ piezoelectric coefficient peak appears near the O to MC transition (the information of average local mode is not shown here), around which $`d_{24}`$ remains larger than 5000 pC/N for a broad range of temperature. The simulations also predict the $`d_{15}`$ peak consistent with the transition from MC to Tri phase. In addition, it is found that with increasing $`\nu `$, the MC-Tri transition temperature decreases, and consequently, the temperature of $`d_{15}`$ peak is dependent on the value of the modulation parameter $`\nu `$. This dependence brings great convenience to developing piezoelectric devices for application at different temperatures.

The above intriguing results can be understood by considering the orientation dependence of dipole-dipole interaction in modulated structures.

Although PbZrO3 and PbTiO3 are similar enough to form Pb(Zr1-xTix)O3 solid solutions at any composition $`x`$, their intrinsic polarization properties are different to some extent. As a result, the magnitude of polarization vibrates with varying local composition that is caused by the structural modulation. In our calculation, the Ti-rich planes have larger average local mode, while Ti-poor planes have smaller values of local mode.

In the homovalent alloys such as PZT, the long-range polarization interactions are described in dipole-dipole interaction energy:WZ ; LB2

$$E_{\mathrm{dipole}}=\frac{Z^2}{ϵ_{\mathrm{}}}\underset{i<j}{}\frac{𝐮_i𝐮_j3(\widehat{𝐑}_{ij}𝐮_i)(\widehat{𝐑}_{ij}𝐮_j)}{R_{ij}^3},$$
(2)
where $`Z^{}`$ is the Born effective charge and $`ϵ_{\mathrm{}}`$ the optical dielectric constant of the material. When the dipole is uniform ($`𝐮_i𝐮`$), $`E_{\mathrm{dipole}}`$ is isotropic,  i.e., $`E_{\mathrm{dipole}}`$ is independent of the direction of the polarization. However, when the magnitude of the dipole fluctuates due to the structural modulation, the situation differs. $`E_{\mathrm{dipole}}`$ becomes dependent on the angle between the directions of modulation and polarization \[see Fig. 4(a)\]: when the polarization is parallel to the modulation, the dipoles are aligned shoulder to shoulder and the energy is higher; when the polarization is perpendicular to the modulation, the dipoles are aligned end to end so that the energy is lower. To further clarify this point, we present a simple numerical analysis here. The local modes in a  plane are assumed to fluctuate as

$$𝐮_i=𝐮[1+\xi K_i],$$
(3)
where $`\xi `$ is the fluctuation amplitude, and $`K_i`$ equals to $`+1`$ or $`1`$ depending on which  plane the dipole locates. It is easy to show that the dipole-dipole interaction energy can be rewritten as

$$E_{\mathrm{dipole}}=E_{\mathrm{dipole}}^0+\xi ^2\mathrm{\Delta }E_{\mathrm{dipole}}.$$
(4)
$`\mathrm{\Delta }E_{\mathrm{dipole}}`$ reflects the variation of dipole energy caused by the structural modulation and relies on the angle between the polarization and the modulation directions (denoted as $`\phi `$). In Fig. 4(b), we plot $`\mathrm{\Delta }E_{\mathrm{dipole}}`$ as a function of $`\phi `$ with polarization rotating from  to  direction. It shows that $`\mathrm{\Delta }E_{\mathrm{dipole}}`$ has its maximum when the polarization is parallel to the modulation direction. When the direction of polarization deviates from that of modulation, $`\mathrm{\Delta }E_{\mathrm{dipole}}`$ continuously decreases and reaches the minimum with polarization perpendicular to the modulation direction. Accordingly, compositional modulation will cause the polarization to rotate away from the modulation direction, which results in unusual structure transitions and induces huge enhancement of piezoelectric coefficient, as revealed in the above case of PZT. In perovskite ultrathin films, the polarization is restricted in the normal direction by the strain from matrix, so the dipole-dipole interaction increases and violates the ferroelectricity below a critical thickness.JJ

It is noted that the structures outside MPB region are not sensitive to the atomic ordering. The main reason is that the dipole-dipole interaction is not the only part to determine the Hamiltonian. When the rotation occurs, the other parts of the Hamiltonian may increase and cause an energy barrier. MPB is a region where different phases have close free energy, which means that the energy barrier of polarization rotation is small. So the dipole-dipole energy dominates in this region and produces the anomalies. When the composition deviates from MPB, such energy barrier increases and the polarization rotation is prevented.

On the basis of the general microscopic mechanism discussed here, it is expected that solid solution made of homovalent perovskite ferroelectrics with a MPB should have the similar structural and piezoelectric anomalies as those of PZT when the atomic ordering is arranged. Besides, compared with heterovalent alloys such as PSN, experimental modifications to the atomic ordering of homovalent alloys such as PZT is more practicable because Pb(Zr1-xTix)O3 is stoichimetric at any $`x`$ value.

This work was supported by State Key Program of Basic Research Development (Grant No. TG2000067108), the National Natural Science Foundation of China, and Trans-century Training Programme Foundation for the Talents by the Ministry of Education of China. W. D. acknowledges with thanks the support of the Berkeley Scholar Program.


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# Gas gain and signal length measurements with a triple-GEM at different pressures of Ar-, Kr- and Xe-based gas mixtures

## 1 Introduction

In the recent years the application range of GEMs (gas electron multipliers)  in detector development has been widened up. Besides the operation in detectors at high energy projects like HERA-B , COMPASS  or DIRAC  the GEM is also used in gaseous photomultiplier development  or X-ray imaging detectors . Thereby, the GEM is usually combined with other micro pattern devices like MSGCs , MGCs , micromegas  or MicroCAT . Also the cascade of multiple GEMs has been tested extensively .

A triple-GEM cascade working as a detector for solar neutrino and dark matter search has been tested at high pressure of pure noble gases . High pressure is also desired in photon detection to increase quantum efficiency. If pure noble gases are not explicitly needed it is helpful to add a quench gas fraction of up to some $`10\%`$ to the noble gases. This leads normally to smaller charge diffusion, shorter signal lengths and the possibility to obtain higher gas gains. Examinations of the gas gaining behaviour of alternative micro pattern devices like MSGCs  or the behaviour of a single GEM/MSGC-combination  in noble gas/quench gas environments show that the maximum gain drops with pressure.

The aim of our investigations is to test the performance of a triple-GEM detector at higher pressures of noble gas/quench gas mixtures to increase the quantum efficiency for photon detection in the energy range of $`8`$$`24\mathrm{keV}`$. We investigate the gas gain behaviour at different pressures and quench gas fractions. We examine the signal lengths which mainly affect the dead time. Besides space charge effects the dead time limits the rate capability.

## 2 Detector setup

The schematic setup of the triple-GEM detector is shown in Fig. 1.

The individual GEM foils with dimensions of $`6\times 6\mathrm{cm}^2`$ are glued under slight tension to a $`1\mathrm{mm}`$ thick ceramic frame. The GEM type is characterised by a hole pitch of $`140\mu \mathrm{m}`$ and an optical transparency of $`12\%`$; the hole shape is double-conical with an inner diameter of about $`50\mu \mathrm{m}`$ and an outer diameter of about $`90\mu \mathrm{m}`$. The holes are hexagonally arranged; the thickness of the GEM amounts to $`60\mu \mathrm{m}`$ including two copper layers of $`5\mu \mathrm{m}`$ each and a Kapton thickness of $`50\mu \mathrm{m}`$.

We have set the distance between the GEMs to $`2\mathrm{mm}`$. The lowermost GEM is mounted at a distance of $`1\mathrm{mm}`$ above the readout structure. Following the usual nomenclature we denote the applied electric field between the GEMs by *transfer field* and the field between the lowermost GEM and the readout structure by *induction field*. Above the GEM configuration a drift cage is mounted which provides a homogeneous *drift field* in the conversion gap of $`27\mathrm{mm}`$.

For the gas gain measurements (s. section 3) a copper anode with a size corresponding to the GEMs has been used. The signal examination (s. section 4) has been carried out with a smaller copper anode ($`1\mathrm{cm}^2`$) to reduce the capacitance and therefore the noise of the preamplifier.

The $`1\mathrm{mm}`$ thick carbon fibre entrance window of the pressure vessel accepts pressures up to about $`3\mathrm{bar}`$. Figs. 24 show the quantum efficiency of a detector filled with $`\text{Ar/CO}_2`$, $`\text{Kr/CO}_2`$ and $`\text{Xe/CO}_2`$ (90/10) with a typical conversion gap of $`25\mathrm{mm}`$.

To achieve high quantum efficiency for photon detection in the energy range of $`5`$$`14\mathrm{keV}`$ xenon gas mixtures are preferably used. For photons in the energy range of about $`14`$$`24\mathrm{keV}`$ quantum efficiency increases by the use of krypton with a K-shell energy of $`14.3\mathrm{keV}`$. Higher quench gas fractions, showed as an example for $`\text{Xe/CO}_2`$ (70/30) in Fig. 4, decrease quantum efficiency.

## 3 Gas gain measurements

In the following section we present results of gas gain measurements in the triple-GEM configuration. The effective gain $`G_{\text{eff}}`$ is experimentally determined by the quotient of the measured current at the anode $`I_{\text{anode}}`$ and the “incoming” current $`I_0`$:

$`G_{\text{eff}}={\displaystyle \frac{I_{\text{anode}}}{I_0}}.`$ (1)
The current

$`I_0=Re{\displaystyle \frac{E_\gamma }{W}}`$ (2)
is determined by the conversion rate $`R`$ of the X-ray photons in counting mode of the detector, by the photon energy $`E_\gamma `$ and by the average energy required to produce one electron-ion pair in the gas $`W`$; $`e`$ denotes the elementary charge.

In fact, the incoming current $`I_0`$ is overestimated – at least at small drift fields and high gas pressures – because of charge losses due to recombination and attachment in the conversion region. This charge loss effect, which is mainly a three-body process and therefore increases with the square of the gas pressure, is shown as an example in Fig. 5

in a $`\text{Xe/CO}_2`$ (90/10) gas mixture at pressures between $`1`$ and $`2\mathrm{bar}`$. At drift fields larger than about $`1000\mathrm{V}/\mathrm{cm}`$ the effective pulse height reaches a plateau. In this region attachment and recombination is negligible and the incoming current $`I_0`$ is described correctly by Eq. (2).

Since the maximum voltage applied to the drift cathode was restricted by the detector geometry to around $`(6000\pm 500)\mathrm{V}`$ we have chosen a drift field of $`400\mathrm{V}/\mathrm{cm}`$ to prevent the detector from sparking at the drift cathode and to have enough margin to increase more crucial potentials like GEM operation voltages. The transfer fields have been chosen to $`2500\mathrm{V}/\mathrm{cm}`$, and we have applied an induction field of $`3000\mathrm{V}/\mathrm{cm}`$ to avoid full discharge propagation . Furthermore, we have set the GEM voltages such, that the uppermost GEM voltage is $`10\%`$ higher than the voltage of the middle GEM; the lowermost GEM is set to an operation voltage $`10\%`$ smaller than the “reference” voltage of the middle GEM $`\mathrm{\Delta }U_{\text{GEM2}}`$. This setting assures minimum discharge rates . The sum of all applied GEM voltages always amounts to $`3\mathrm{\Delta }U_{\text{GEM2}}`$.

For illumination with X-ray photons we have used a $`{}_{}{}^{55}\text{Fe}`$ source, emitting photons with an energy of $`5.9\mathrm{keV}`$ and with a rate of $`41\mathrm{kHz}`$ collimated to about $`28\mathrm{mm}^2`$. During all measurements the gas gain was found to decrease as a function of illumination time and photon rate most likely due to charging of the insulating Kapton in the GEM. The charging is dependent on illumination time and position, photon flux and dryness of the Kapton surface. We can not explain why in our setup the gain decreased as a function of time, whereas gain increased in measurements of other groups (i.e. ,). The problem of charging of the Kapton and hence of the time and rate dependent gas gaining behaviour may be solved by using carbon coated gas electron multipliers . In our case, however, all data has been taken after an equilibrium state had been reached.

The gas gain measurements were limited by sparks. We stopped the measurements at spark rates $`2\mathrm{sparks}/\mathrm{min}`$, which is rather an arbitrary limit. Important, however, is the stable detector operation at slightly lower voltages and hence lower gas gains.

### 3.1 Gas gain in $`\text{Ar/CO}_2`$ (70/30)

Although quantum efficiency in argon mixtures for photon detection in the higher energy range is small compared to krypton or xenon mixtures we have carried out gas gain measurements in $`\text{Ar/CO}_2`$ (70/30) to compare the results to those achieved with Kr- and Xe-mixtures. The measured effective gain, shown in Fig. 6,

exceeds $`610^4`$ at standard pressure. The maximum gas gain achievable decreases with pressure, but we have still obtained a maximum gain of about $`10^4`$ at a pressure of $`3\mathrm{bar}`$.

### 3.2 Gas gain in $`\text{Kr/CO}_2`$ mixtures

We have investigated two Kr-mixtures with different $`\text{CO}_2`$ fractions of $`30\%`$ (see Fig. 7)

and $`10\%`$ (see Fig. 8),

respectively. In both mixtures the effective gain exceeds $`10^4`$ up to pressures of $`2\mathrm{bar}`$. Nevertheless, a quench gas fraction of $`30\%`$ is not well suited for operation at pressures $`>2\mathrm{bar}`$ where we obtained a strong decrease in gas gain to about $`200`$. In contrast to that still large gas gains in the order of $`510^3`$ are possible with a carbon dioxide fraction of $`10\%`$.

### 3.3 Gas gain in $`\text{Xe/CO}_2`$ mixtures

The use of Xe-based gas mixtures offers the largest quantum efficiency for photon detection in the energy range between $`5`$ and $`14\mathrm{keV}`$. Results of gas gain measurements for $`\text{Xe/CO}_2`$ (70/30) and $`\text{Xe/CO}_2`$ (90/10) are shown in Fig. 9

and Fig. 10.

Like for Kr-gas mixtures an amount of $`10\%`$ carbon dioxide enables operation with gas gains $`>10^3`$ at pressures above $`2\mathrm{bar}`$. High quencher fractions are not well suited for pressure operation with xenon.

### 3.4 Homogeneity

Figure 11

shows the relative effective gain measured along the vertically centred $`x`$-axis. Gain variations of up to $`25\%`$ become obvious. These local variations are mainly due to two aspects: First, the GEMs, themselves, produce intrinsic gain inhomogeneities because of geometry variations. Furthermore, the distances between the individual GEMs and the distance between undermost GEM and anode are not constant over all the detector area, which leads to transfer and induction field inhomogeneities und finally to variations in the charge transfer behaviour and in the effective gas gain of the GEMs .

### 3.5 Discussion

We have measured the gas gain behaviour at different pressures of argon, krypton and xenon with additions of $`10\%`$ and $`30\%`$ of carbon dioxide. A strong influence of the quench gas fraction on the gas gain behaviour becomes obvious. It is definitely a non-trivial task to optimise the fraction of quencher at a given pressure with respect to a maximum achievable gain due to a complicated interplay of these parameters.

Generally, the maximum gas gain of the triple-GEM achievable in slightly quenched noble gas mixtures is higher than in pure noble gases (compare to Refs. ). At standard pressure the krypton and xenon gas mixtures with $`10\%`$ $`\text{CO}_2`$ behave relatively similarly to the mixtures with $`30\%`$ $`\text{CO}_2`$. Increasing gas pressure leads to a larger deviation in maximum achievable gas gain. Higher pressure demands obviously for smaller quench gas fractions.

The strong influence of the quencher fraction indicates, that a stable avalanche process is not only based on electron-induced ionization of gas atoms. The UV-photons which are produced in the avalanche development may contribute noticeably to the multiplication procedure. With increasing pressure and constant (or even larger) quench gas fraction the mean free path of the UV-photons is decreasing. For instance, the deterioration in energy resolution in a MWPC is stopped when a very small quench gas fraction of only $`2\%`$ at very high pressures (up to $`30\mathrm{bar}`$) is added to argon . However, still smaller fractions of quenching gas lead to an unsafe operation of the detector. We suppose, that the triple-GEM detector shows a comparable behaviour. It should be considered to use very small quench gas fractions of a few percent for really high pressure operation.

A good choice for photon detection with the triple-GEM is the use of $`\text{Kr/CO}_2`$ or $`\text{Xe/CO}_2`$ (90/10), depending on the energy range, at pressures between $`1`$ and $`2\mathrm{bar}`$. Gas gains of $`510^3`$ can be easily reached without sparking.

## 4 Signal length investigations

We have studied the dependence of the anode signal shape on GEM voltage, induction field, transfer field and drift field for all gas mixtures and several pressures since the dead time behaviour of the detector is mainly determined by the signals lengths. The copper readout anode for these measurements has a size of $`1\times 1\mathrm{cm}^2`$. The integrating preamplifier and the shaper including a pole-zero filter to cancel the pole of the integrating first stage are in-house developments. The gaussian-like $`\delta `$-response of this amplification system has a width of $`15\mathrm{ns}`$ (fwhm) due to bandwidth limitations.

Basically, the anode signal shape is determined by two aspects:

1. A spatially $`\delta `$-like distributed electron cluster moving from the bottom side of the undermost GEM towards the readout structure induces a box-shaped current at both involved electrodes if the electric field and therefore the electron drift velocity in the region of interest is assumed to be constant . The copper-clad bottom side of the GEM shields all currents induced by charge movements appearing above this electrode; especially the slow ions do not contribute to the signal shape, which is, however, the case for micromegas or MicroCAT detectors . The crucial parameters for the width $`t_\text{w}`$ of the box-shaped current are the electron drift velocity $`v_\text{e}`$ in the electric field of the induction region and the distance $`d`$ between the bottom side of the GEM and the anode which amounts to $`1\mathrm{mm}`$ in our case:

$`t_\text{w}={\displaystyle \frac{d}{v_\text{e}}}.`$ (3)
2. The longitudinal diffusion $`\sigma _\text{l}`$ of the primary produced electrons (photoelectron plus subsequently produced about 300 electrons for $`8\mathrm{keV}`$ photons in argon) in the conversion region leads to a temporal gaussian smearing of the above mentioned box function, mathematically expressed by a convolution of box and gauss function. The width of the gaussian

$`\sigma _\text{t}=\left(\sigma _{\text{l0}}\overline{\sqrt{l}}\right)/v_\text{e}`$ (4)
is determined by the longitudinal diffusion coefficient $`\sigma _{\text{l0}}`$ and the electron drift velocity $`v_\text{e}`$ in the applied drift field and gas mixture used and finally by the mean drift path $`\left(\overline{\sqrt{l}}\right)^2`$ of the primary produced electrons, which is dependent on photon energy, conversion gap and photoelectric absorption coefficient of the gas. Additionally, the longitudinal electron diffusion in the two transfer regions between the GEMs and in the induction region between undermost GEM and anode contribute to the temporal smearing $`\sigma _\text{t}`$. In our simulation this contribution has also been taken into account.

For most gas mixtures and pressures in our detector setup the temporal diffusion spreading (compare to Eq. (4)) is the main contribution which leads to a very much gaussian-like signal shape. Fig. 12

shows a typical signal obtained at a high drift field of $`1000\mathrm{V}/\mathrm{cm}`$ at standard pressure. At smaller drift fields the signal shape looks differently (s. Fig. 13).

The signal shape is not continuous anymore; single electron clusters reach the anode one by one, but still the gaussian character is well visible. We have measured the full width half maximum (fwhm) of the anode signals and the $`\delta `$-response of the preamplifier with a digital oscilloscope, afterwards averaging the widths of several signals.

Due to the gaussian signal shape and the gaussian $`\delta `$-response of the preamplifier/shaper-system the real signal length can be calculated to be the width of the deconvolution of both gaussians:

$`\mathrm{\Delta }_{\text{sig-real}}^2=\mathrm{\Delta }_{\text{sig-meas}}^2\mathrm{\Delta }_{\delta \text{-response}}^2,`$ (5)
where $`\mathrm{\Delta }`$ is the full width half maximum of the signal. In case the measured signal shape is not gaussian (which means that the main contribution of the signal is due to the electron induced box-shaped current, which is true for very small induction fields (s. section 4.2)) Eq. (5) is no longer valid. But in this case the measured signal width is very much larger than the width of the $`\delta `$-response ($`\mathrm{\Delta }_{\text{sig-meas}}\mathrm{\Delta }_{\delta \text{-response}}`$) and therefore the real signal width can be determined to be $`\mathrm{\Delta }_{\text{sig-real}}\mathrm{\Delta }_{\text{sig-meas}}`$.

Despite most gas properties are $`E/p`$-dependent all measurements have been performed with a constant transfer field of $`2500\mathrm{V}/\mathrm{cm}`$ and a constant induction field of $`3000\mathrm{V}/\mathrm{cm}`$ even at high pressure if not noted otherwise, since these electric fields ensure maximum electron transparency of the GEM. The $`{}_{}{}^{55}\text{Fe}`$ source has been collimated to about $`12\mathrm{mm}^2`$; photons were emitted with a rate of a few hundred $`\mathrm{Hz}`$. We have carried out all signal width simulations only for $`1\mathrm{bar}`$ $`\text{Ar/CO}_2`$ (70/30), where experimental data on drift velocities  and simulated data on longitudinal diffusion  have been used.

### 4.1 Influence of GEM operation voltage

We have detected no influence of the GEM voltage on the signal length. The range of the investigated GEM voltages was limited by the dynamic range of the preamplifier. Anyway, the setting of the GEM voltage is determined by the desired gas gain and is therefore no freely adjustable parameter for optimisation of the signal lengths.

### 4.2 Influence of the induction field

The contribution of the width of the box-shaped current to the total width of the signal increases for very small induction fields due to a decreasing electron drift velocity (compare to Eq. (3)). Three-dimensional field calculations with Maxwell  using a geometry of $`1\mathrm{mm}`$ transfer gap, the $`60\mu \mathrm{m}`$ thick GEM foil and $`1\mathrm{mm}`$ induction gap (the geometry of the GEM and more simulation details are described in Ref. ) show that the electric field in the induction region along the symmetry axis of a GEM hole is larger than the quotient $`E=U_{\text{GEM-bottom}}/d`$ of the applied voltage on the bottom side of the GEM $`U_{\text{GEM-bottom}}`$ and the distance $`d`$ between GEM bottom and anode. This effect is some relict due to the very high electric field in the holes. To determine the width of the electron induced box-shaped current we have used a parametrisation of the electron drift velocity, calculated by the Magboltz programm , up to electric fields of $`20\mathrm{kV}/\mathrm{cm}`$. An average drift velocity in the induction region has been calculated and the box function is convoluted with a gaussian, describing the diffusion spreading. The results of this simulation and the comparison to experiment is shown in Fig. 14.

A good agreement especially for induction fields $`1\mathrm{kV}/\mathrm{cm}`$ becomes obvious. At induction fields larger than about $`2000\mathrm{V}/\mathrm{cm}`$ the influence of the box-shaped current becomes negligible compared to the contribution of the temporal electron diffusion in the conversion region.

### 4.3 Influence of the transfer field

For this study both transfer fields between GEM1 and GEM2 and between GEM2 and GEM3 have been changed at the same time. The measured results are shown in Fig. 15.

Transfer fields smaller than $`2500\mathrm{V}/\mathrm{cm}`$ result in a slight increase of the signal width which can be explained by smaller electron drift velocities in the transfer regions and hence a larger diffusion spreading (compare to Eq. (4)). At larger transfer fields the signal width reaches a plateau. Higher pressure reflects smaller electron drift velocities and therefore larger signal widths.

### 4.4 Influence of the drift field

This section contains an intensive investigation of the influence of the applied drift field on the signal width. The comparison between measurement and simulation (see Fig. 16)

shows a good agreement for drift fields $`200\mathrm{V}/\mathrm{cm}`$. The signal width measurements at small drift fields are very difficult due to the clustered signal shape (see Fig. 13). Therefore, the error is relatively large when determining these signal lengths. Furthermore, a large part of the primary produced electrons is lost due to recombination and attachment at low drift fields (compare to Fig. 5) and thus decreasing the signal-to-noise ratio.

The measured signal widths for different gas mixtures and gas pressures are shown in Figs. 1721.

Generally, high drift fields are needed to produce short signals. We were limited to about $`1000`$$`1200\mathrm{V}/\mathrm{cm}`$ due to sparking at the drift cathode. The fastest signals with a signal length of $`<25\mathrm{ns}`$ (fwhm) are produced in the argon mixture at standard pressure (see Fig. 17). Larger pressure always increases the signal width due to decreasing drift velocities in induction and conversion region and thus an increasing temporal smearing. But even in $`1.5\mathrm{bar}`$ $`\text{Xe/CO}_2`$ (90/10) the signal width does not exceed $`60\mathrm{ns}`$ (fwhm) at a drift field of $`1100\mathrm{V}/\mathrm{cm}`$.

### 4.5 Discussion

In our detector setup the drift field has the most crucial influence on the signal length although for smaller conversion regions this parameter becomes less important due to smaller longitudinal electron diffusion. The drift field should be chosen as large as allowed by the detector setup. However, the drift field should not be too high ($`2\mathrm{kV}/\mathrm{cm}`$) because the uppermost GEM loses transparency for too large drift fields . Transfer and induction fields $`2\mathrm{kV}/\mathrm{cm}`$ minimise the widths of the signal. If, however, the contribution of the electron induced box-shaped current becomes noticeable the distance between the undermost GEM and the anode can be reduced, i.e. to $`0.5\mathrm{mm}`$. This should suppress this effect. The GEM operation voltage, which is mainly determined by the desired gas gain, does not influence the signal widths visibly.

## 5 Conclusion

We have measured the gas gain in a triple-GEM geometry for pressures up to $`3\mathrm{bar}`$ of $`\text{Ar/CO}_2`$ (70/30), $`\text{Kr/CO}_2`$ (70/30), $`\text{Kr/CO}_2`$ (90/10), $`\text{Xe/CO}_2`$ (70/30) and $`\text{Xe/CO}_2`$ (90/10). At a pressure $`>2\mathrm{bar}`$ the addition of $`10\%`$ of carbon dioxide to the noble gases leads to higher maximum gas gains compared to noble gases mixed with $`30\%`$ quench gas. Too large amounts of quench gas seem to disturb operation at high pressure and is therefore not preferable. Generally, we have obtained that the quench gas fraction should decrease with pressure.

Compared to the geometry of MicroCAT- or micromegas-detectors the triple-GEM-detector offers faster signals since only the electrons and not the slow ions contribute to the signal shape at the anode. The measured signal lengths at high drift fields in all gas mixtures and pressures investigated are smaller than about $`100\mathrm{ns}`$ (fwhm). If transfer and induction fields exceed $`2\mathrm{kV}/\mathrm{cm}`$ the signal widths get to minimum.

Provided that the signal width is mainly determined by the temporal diffusion of the primary electrons in the conversion region further optimisation with respect to an increased high rate behaviour can be performed with exact knowledge of photon energy and desired quantum efficiency by reducing the conversion gap (compare to Figs. 24). For example, with a desired quantum efficiency of $`90\%`$ for $`8\mathrm{keV}`$-photons in $`1.5\mathrm{bar}`$ $`\text{Xe/CO}_2`$ (90/10) it is sufficient to provice a conversion gap of $`11\mathrm{mm}`$ with mean drift path $`\left(\overline{\sqrt{l_{11}}}\right)^2`$ instead of $`27\mathrm{mm}`$ with mean drift path $`\left(\overline{\sqrt{l_{27}}}\right)^2`$ used the for measurements described in this paper. Hence, the longitudinal diffusion and consequently the signal width will decrease by a factor of $`\overline{\sqrt{l_{27}}}/\overline{\sqrt{l_{11}}}1.8`$.

In combination with the resistive readout structure  it is proposed to integrate about $`90\%`$ of the charge to achieve optimum spatial resolution . Compared to the signal length fwhm, presented here, the charge integration time from $`5\%`$ to $`95\%`$ of the original signal can be calculated to be $`\tau _{595\%}1.4\tau _{\text{fwhm}}`$. Due to charge diffusion on the readout structure the charge integration time for signals with a width of $`\tau _{\text{5-95\hspace{0.17em}\%}}=92\mathrm{ns}`$ is stretched to about $`\tau _{\text{rs:5-95\hspace{0.17em}\%}}=150\mathrm{ns}`$.

We are grateful to the inner tracker group of the HERA-B collaboration for providing several GEM foils. We thank C. Fiorini for providing the preamplifier design.


text:
# A generalized mean value inequality for subharmonic functions and applications

## 1. Introduction

### 1.1 Previous results

If $`u`$ is a nonnegative and subharmonic function on $`\mathrm{\Omega }`$ and $`p>0`$, then there is a constant $`C=C(n,p)1`$ such that

(1)
$$u(x)^p\frac{C}{m(B(x,r))}_{B(x,r)}u(y)^p𝑑m(y)$$

for all $`B(x,r)\mathrm{\Omega }`$. Here $`\mathrm{\Omega }`$ is a domain in $`^n`$, $`n2`$, $`B(x,r)`$ is the Euclidean ball with center $`x`$ and radius $`r`$, and $`m`$ is the Lebesgue measure in $`^n`$. See \[FeSt72, Lemma 2, p. 172\], \[Ku74, Theorem 1, p. 529\], \[Ga81, Lemma 3.7, pp. 121-123\], \[AhRu93, (1.5), p. 210\]. These authors considered only the case when $`u=|v|`$ and $`v`$ is harmonic function. However, the proofs in \[FeSt72\] and \[Ga81\] apply verbatim also in the general case of nonnegative subharmonic functions. This was pointed out in \[Ri89, Lemma, p. 69\], \[Su90, p. 271\], \[Su91, p. 113\], \[Ha92, Lemma 1, p. 113\], \[Pa94, p. 18\] and \[St98, Lemma 3, p. 305\]. In \[AhBr88, p. 132\] it was pointed out that a modification of the proof in \[FeSt72\] gives in fact a slightly more general result, see 2.1 below. A possibility for an essentially different proof was pointed out already in \[To86, pp. 188-190\]. Later other different proofs were given in \[Pa94, p. 18, and Theorem 1, p. 19\] (see also \[Pa96, Theorem A, p. 15\]), \[Ri99, Lemma 2.1, p. 233\] and \[Ri01,Theorem, p. 188\]. The results in \[Pa94\], \[Ri99\] and \[Ri01\] hold in fact for more general function classes than just for nonnegative subharmonic functions. See 2.1 and Theorem A below. Compare also \[DBTr84\] and \[Do88, p. 485\].

The inequality $`(1)`$ has many applications. Among others, it has been applied to the (weighted) boundary behavior of nonnegative subharmonic functions \[To86, p. 191\], \[Ha92, Theorems 1 and 2, pp. 117-118\], \[St98, Theorems 1, 2 and 3, pp. 301, 307\], \[Ri99, Theorem, p. 233\] and on the nonintegrability of subharmonic and superharmonic functions \[Su90, Theorem 2, p. 271\], \[Su91, Theorem, p. 113\].

Because of the importance of the mean value inequality $`(1)`$, it is worthwhile to present a unified result which contains this mean value inequality and all its generalizations cited above. Below in Theorem 2.5 we propose such a generalization. Instead of nonnegative subharmonic functions we formulate our result slightly more generally for functions which we call *quasi-nearly subharmonic functions* and which will be defined in 2.1. We also give two applications.

As the first application we improve in Theorem 3.4 below our recent result \[Ri99, Theorem, p. 233\] on the weighted boundary behavior of nonnegative subharmonic functions. As the second application we give in Corollary 4.5 below a supplement to Suzuki’s results on the nonintegrability of superharmonic and subharmonic functions \[Su91, Theorem, p. 113\]. Our result is a limiting case to Suzuki’s results.

### 1.2 Notation

Our notation is more or less standard, see \[Ri99\]. However, for convenience of the reader we recall here the following. We use the common convention $`0\mathrm{}=0`$. We write $`\nu _n=m(B(0,1))`$. The $`d`$-dimensional Hausdorff (outer) measure in $`^n`$ is denoted by $`H^d`$, $`0dn`$. In the sequel $`\mathrm{\Omega }`$ is always a domain in $`^n`$, $`\mathrm{\Omega }^n`$, $`n2`$. The diameter of $`\mathrm{\Omega }`$ is denoted by diam $`\mathrm{\Omega }`$. The distance from $`x\mathrm{\Omega }`$ to $`\mathrm{\Omega }`$, the boundary of $`\mathrm{\Omega }`$, is denoted by $`\delta (x)`$. $`_{\mathrm{loc}}^1(\mathrm{\Omega })`$ is the space of locally integrable functions on $`\mathrm{\Omega }`$. Our constants $`C`$ are always positive, mostly $`1`$, and they may vary from line to line.

## 2. Quasi-nearly subharmonic functions

### 2.1 The definition

We call a (Lebesgue) measurable function $`u:\mathrm{\Omega }[\mathrm{},\mathrm{}]`$ quasi-nearly subharmonic, if $`u_{\text{loc}}^1(\mathrm{\Omega })`$ and if there is a constant $`C_0=C_0(n,u,\mathrm{\Omega })1`$ such that

(2)
$$u(x)\frac{C_0}{r^n}_{B(x,r)}u(y)𝑑m(y)$$

for any ball $`B(x,r)\mathrm{\Omega }`$. Compare \[Ri99, p. 233\] and \[Do57, p. 430\]. Nonnegative quasi-nearly subharmonic functions have previously been considered by \[Pa94\] (he called them "functions satisfying the shK-condition") and in \[Ri99\] (where they were called "pseudosubharmonic functions"). See \[Do88, p. 485\] for an even more general function class of (nonnegative) functions. As a matter of fact, also we will restrict ourselves to nonnegative functions.

Nearly subharmonic functions, thus also quasisubharmonic and subharmonic functions, are examples of quasi-nearly subharmonic functions. Recall that a function $`u_{\text{loc}}^1(\mathrm{\Omega })`$ is nearly subharmonic, if $`u`$ satisfies $`(2)`$ with $`C_0=\frac{1}{\nu _n}`$. See \[Her71, pp. 14, 26\]. Furthermore, if $`u0`$ is subharmonic and $`p>0`$, then by $`(1)`$ above, $`u^p`$ is quasi-nearly subharmonic. By \[Pa94, Theorem 1, p. 19\] or \[Ri99, Lemma 2.1, p. 233\] this holds even if $`u0`$ is quasi-nearly subharmonic. See also \[AhBr88, p. 132\].

### 2.2 Permissible functions

In \[Ri01, Theorem, p. 188\] we proved the following result which contains essentially the cited results in \[Pa94\] and \[Ri99\] as special cases.

Theorem A. (\[Ri01, Theorem, p. 188\]) *Let $`u`$ be a nonnegative subharmonic function on $`\mathrm{\Omega }`$. Let $`\psi :_+_+`$ be a concave surjection whose inverse $`\psi ^1`$ satisfies the $`\mathrm{\Delta }_2`$-condition. Then there exists a constant $`C=C(n,\psi ,u)1`$ such that*

$$\psi (u(x_0))\frac{C}{\varrho ^n}_{B(x_0,\varrho )}\psi (u(y))𝑑m(y)$$

*for any ball $`B(x_0,\varrho )\mathrm{\Omega }`$.*

Recall that a function $`\psi :_+_+`$ satisfies the $`\mathrm{\Delta }_2`$-condition, if there is a constant $`C=C(\psi )1`$ such that

$$\psi (2t)C\psi (t)$$

for all $`t_+`$.

In order to improve our result, Theorem A above, still further, we give the following definition. A function $`\psi :_+_+`$ is permissible, if there is a nondecreasing, convex function $`\psi _1:_+_+`$ and an increasing surjection $`\psi _2:_+_+`$ such that $`\psi =\psi _2\psi _1`$ and such that the following conditions are satisfied:

* $`\psi _1`$ satisfies the $`\mathrm{\Delta }_2`$-condition.
* $`\psi _2^1`$ satisfies the $`\mathrm{\Delta }_2`$-condition.
* The function $`t\frac{t}{\psi _2(t)}`$ is quasi-increasing, i.e. there is a constant $`C=C(\psi _2)1`$ such that

$$\frac{s}{\psi _2(s)}C\frac{t}{\psi _2(t)}$$

for all $`s,t_+`$, $`0st`$.

Observe that the condition (b) is equivalent with the following condition.

* For some constant $`C=C(\psi _2)1`$,

$$\psi _2(Ct)2\psi _2(t)$$

for all $`t_+`$.

If $`\psi `$ is a permissible function, we will in the sequel use always one, fixed constant $`C_1=C_1(\psi )`$, in the case of all the properties (a), (b), (c) (and (b’)). If $`\psi :_+_+`$ is an increasing surjection satisfying the conditions (b) and (c), we say that it is strictly permissible. Permissible functions are necessarily continuous.

Let it be noted that the condition (c) above is indeed natural. For just one counterpart to it, see e.g. \[HiPh57, Theorem 7.2.4, p. 239\].

Observe that our previous definition for permissible functions in \[Ri99, 1.3, p. 232\] was *much more restrictive*: A function $`\psi :_+_+`$ was there defined to be *permissible* if it is of the form $`\psi (t)=\vartheta (t)^p`$, $`p>0`$, where $`\vartheta :_+_+`$ is a nondecreasing, convex function satisfying the $`\mathrm{\Delta }_2`$-condition.

2.3 Remarks The following list gives examples of permissible functions (we leave the slightly tedious verifications to the reader). Our list, especially (ii), shows that the considered class of permissible functions is wide and natural. On the other hand, in view of the simple example in (vi), one sees that functions of type (ii) are by no means the only permissible functions: There exists a huge amount of permissible functions of other types.

* The functions $`\psi _1(t)=\vartheta (t)^p`$, $`p>0`$, already considered in \[Ri99, (1.3), p. 232, and Lemma 2.1, p. 233\].
* Functions of the form $`\psi _2=\varphi _2\phi _2`$, where $`\varphi _2:_+_+`$ is a concave surjective function whose inverse $`\varphi _2^1`$ satisfies the $`\mathrm{\Delta }_2`$-condition, and $`\phi _2:_+_+`$ is a nondecreasing convex function satisfying the $`\mathrm{\Delta }_2`$-condition. (Observe here that any concave function $`\varphi _2:_+_+`$ is necessarily nondecreasing.) These (or, to be more exact, the functions $`\varphi _2`$ defined above) were considered in \[Ri01, Theorem, p. 188\].
* $`\psi _3(t)=ct^{p\alpha }[\mathrm{log}(\delta +t^{p\gamma })]^\beta `$, where $`c>0`$, $`0<\alpha <1`$, $`\delta 1`$, and $`\beta ,\gamma `$ are such that $`0<\alpha +\beta \gamma <1`$, and $`p1`$.
* For $`0<\alpha <1`$, $`\beta 0`$ and $`p1`$,

$$\psi _4(t)=\{\begin{array}{cc}p^\beta t^{p\alpha },\hfill & \text{ for }0te,\hfill \\ t^{p\alpha }(\mathrm{log}t^p)^\beta ,\hfill & \text{ for }t>e.\hfill \end{array}$$
* For $`0<\alpha <1`$, $`\beta <0`$ and $`p1`$,

$$\psi _5(t)=\{\begin{array}{cc}(\frac{\beta p}{\alpha })^\beta t^{p\alpha },\hfill & \text{ for }0te^{\beta /\alpha },\hfill \\ t^{p\alpha }(\mathrm{log}t^p)^\beta ,\hfill & \text{ for }t>e^{\beta /\alpha }.\hfill \end{array}$$
* For $`p1`$,

$$\psi _6(t)=\{\begin{array}{ccc}2n+\sqrt{t^p2n},\hfill & \text{ for }t^p[2n,2n+1),\hfill & n=0,1,2,\mathrm{},\hfill \\ 2n+1+[t^p(2n+1)]^2,\hfill & \text{ for }t^p[2n+1,2n+2),\hfill & n=0,1,2,\mathrm{}.\hfill \end{array}$$

For $`p=1`$ the functions in (i), (iii), (iv), (v), (vi), and also in (ii) provided $`\phi _2(t)=t`$, are strictly permissible.

2.4 Remark. Our previous results were restricted to the cases where $`\psi `$ was either of type (i) (\[Ri99, (1.3), p. 232, and Lemma 2.1, p. 233\]) or of type (ii) (\[Ri01, Theorem, p. 188\] (or Theorem A above)). Now we give a refinement to our results in a unified form. The proof is a modification of Pavlović’s argument \[Pa94, proof of Theorem 1, p. 20\].

2.5 Theorem. *Let $`u`$ be a nonnegative quasi-nearly subharmonic function on $`\mathrm{\Omega }`$. If $`\psi :_+_+`$ is a permissible function, then $`\psi u`$ is quasi-nearly subharmonic on $`\mathrm{\Omega }`$.*

Proof. In view of \[Ri99, Lemma 2.1, p. 233\] we may restrict us to the case where $`\psi =\psi _2:_+_+`$ is strictly permissible.

Since $`\psi `$ is continuous, $`\psi u`$ is measurable and $`\psi u_{\text{loc}}^1(\mathrm{\Omega })`$. It remains to show that $`\psi u`$ satisfies the generalized mean value inequality (2). But this can be seen exactly as in \[Ri01, proof of Theorem, pp. 188-189\], the only difference being that instead of the property 2.4 in \[Ri01, p. 188\] of concave functions, one now uses the above property (c) in 2.2 of permissible functions. $`\mathrm{}`$

## 3. Weighted boundary behavior

### 3.1 Stoll’s result.

Improving previous results of Gehring \[Ge57, Theorem 1, p. 77\] and Hallenbeck \[Ha92, Theorems 1 and 2, pp. 117-118\], Stoll \[St98, Theorem 2, p. 307\] gave the following result.

Theorem B.  *Let $`f`$ be a nonnegative subharmonic function on a domain $`G`$ in $`^n`$, $`G^n`$, $`n2`$, with $`𝒞^1`$ boundary. Let*

(3)
$$_Gf(x)^p\delta (x)^\gamma 𝑑m(x)<\mathrm{}$$

*for some $`p>0`$ and $`\gamma >1\beta (p)`$. Let $`0<dn1`$. Then for each $`\tau 1`$ and $`\alpha >0`$ ($`\alpha >1`$ when $`\tau =1`$), there exists a subset $`E_\tau `$ of $`G`$ with $`H^d(E_\tau )=0`$ such that*

$$\underset{\rho 0}{lim}\{\underset{x\mathrm{\Gamma }_{\tau ,\alpha ,\rho }(\zeta )}{sup}[\delta (x)^{n+\gamma \frac{d}{\tau }}f(x)^p]\}=0$$

*for all $`\zeta GE_\tau `$.*

Above, for $`\zeta G`$ and $`\varrho >0`$,

$$\mathrm{\Gamma }_{\tau ,\alpha ,\varrho }(\zeta )=\mathrm{\Gamma }_{\tau ,\alpha }(\zeta )G_\varrho ,$$

where

$$\mathrm{\Gamma }_{\tau ,\alpha }(\zeta )=\{xG:|x\zeta |^\tau <\alpha \delta (x)\},G_\varrho =\{xG:\delta (x)<\varrho \}.$$

Moreover, $`\beta (p)=\mathrm{max}\{(n1)(1p),0\}`$. Stoll makes the assumption $`\gamma >1\beta (p)`$ in order to exclude the trivial case $`f0`$. As a matter of fact, it follows from a result of Suzuki \[Su90, Theorem 2, p. 271\] that $`(3)`$ together with the condition $`\gamma 1\beta (p)`$ implies indeed that $`f0`$, provided $`G`$ is a bounded domain with $`𝒞^2`$ boundary.

Our previous improvement \[Ri99, Theorem, p. 233\] to Stoll’s result, Theorem B above, can now be refined slightly further, just using our above result Theorem 2.5. This refinement will be given in Theorem 3.4 below. For this purpose we first recall, and just for the convenience of the reader, some terminology from \[Ri99, pp. 231–232\].

### 3.2 Admissible functions

A function $`\phi :_+_+`$ is admissible, if it is increasing (strictly), surjective, and there are constants $`C_2>1`$ and $`r_2>0`$ such that

(4)
$$\phi (2t)C_2\phi (t)\text{ and}\phi ^1(2s)C_2\phi ^1(s)\text{for all}s,t_+,\mathrm{\hspace{0.17em}\hspace{0.17em}0}s,tr_2.$$

Nonnegative, nondecreasing functions $`\phi _1(t)`$ which satisfy the $`\mathrm{\Delta }_2`$-condition and for which the functions $`t\frac{\phi _1(t)}{t}`$ are nondecreasing, are examples of admissible functions. Further examples are $`\phi _2(t)=ct^\alpha [\mathrm{log}(\delta +t^\gamma )]^\beta ,`$ where $`c>0`$, $`\alpha >0`$, $`\delta 1`$, and $`\beta ,\gamma `$ are such that $`\alpha +\beta \gamma >0`$.

### 3.3 Accessible boundary points and approach regions

Let $`\phi :_+_+`$ be an admissible function and let $`\alpha >0`$. We say that $`\zeta \mathrm{\Omega }`$ is $`(\phi ,\alpha )`$-accessible, if

$$\mathrm{\Gamma }_\phi (\zeta ,\alpha )B(\zeta ,\rho )\mathrm{}$$

for all $`\rho >0`$. Here

$$\mathrm{\Gamma }_\phi (\zeta ,\alpha )=\{x\mathrm{\Omega }:\phi (|x\zeta |)<\alpha \delta (x)\},$$

and we call it a $`(\phi ,\alpha )`$-approach region in $`\mathrm{\Omega }`$ at $`\zeta `$.

Mizuta \[Mi91\] has considered boundary limits of harmonic functions in Sobolev-Orlicz classes on bounded Lipschitz domains $`U`$ of $`^n`$, $`n2`$. His approach regions are of the form

$$\mathrm{\Gamma }_\varphi (\zeta ,\alpha )=\{xU:\varphi (|x\zeta |)<\alpha \delta (x)\},$$

where now $`\varphi :_+_+`$ is a nondecreasing function which satisfies the $`\mathrm{\Delta }_2`$-condition and is such that $`t\frac{\varphi (t)}{t}`$ is nondecreasing. As pointed out above, such functions are admissible in our sense. In fact, they form a proper subclass of our admissible functions.

3.4 Theorem. *Let $`H^d(\mathrm{\Omega })<\mathrm{}`$ where $`0dn`$. Suppose that $`u`$ is a nonnegative quasi-nearly subharmonic function in $`\mathrm{\Omega }`$. Let $`\phi :_+_+`$ be an admissible function and $`\alpha >0`$. Let $`\psi :_+_+`$ be a permissible function. Suppose that*

(5)
$$_\mathrm{\Omega }\psi (u(x))\delta (x)^\gamma 𝑑m(x)<\mathrm{}$$

*for some $`\gamma `$. Then*

$$\underset{\rho 0}{lim}(\underset{x\mathrm{\Gamma }_{\phi ,\rho }(\zeta ,\alpha )}{sup}\{\delta (x)^{n+\gamma }[\phi ^1(\delta (x))]^d\psi (u(x))\})=0$$

*for $`H^d`$-almost every $`(\phi ,\alpha )`$-accessible point $`\zeta \mathrm{\Omega }`$. Here*

$$\mathrm{\Gamma }_{\phi ,\rho }(\zeta ,\alpha )=\{x\mathrm{\Gamma }_\phi (\zeta ,\alpha ):\delta (x)<\rho \}.$$

The proof is verbatim the same as \[Ri99, proof of Theorem, pp. 235–238\], except that now we just replace \[Ri99, Lemma 2.1, p. 233\] by the more general Theorem 2.5 above.  ∎

3.5 Remark. Unlike Stoll, we have imposed no restrictions on the exponent $`\gamma `$ in order to exclude the trivial case $`u0`$. We refer, however, to such possibilities in Remark 4.7 below, after having given in Corollary 4.5 a limiting case result for a result of Suzuki.

## 4. A Limiting case result to nonintegrability results of Suzuki

### 4.1 Suzuki’s result

Suzuki \[Su91, Theorem and its proof, pp. 113–115\] gave the following result.

Theorem C. *Let $`0<p1`$. If a superharmonic (resp. nonnegative subharmonic) function $`v`$ on $`\mathrm{\Omega }`$ satisfies*

(6)
$$_\mathrm{\Omega }|v(x)|^p\delta (x)^{npn2p}𝑑m(x)<\mathrm{},$$

*then $`v`$ vanishes identically.*

Suzuki pointed also out that his result is sharp in the following sense: If $`p`$, $`0<p1`$, is fixed, then the exponent $`\gamma =npn2p`$ cannot be increased. On the other hand, clearly $`n<\gamma 2`$, when $`0<p1`$. Since the class of permissible functions include, in addition the functions $`t^p`$, $`0<p1`$, also a large amount of essentially different functions (see 2.3 above), one is tempted to ask whether there exists any limiting case result for Suzuki’s results, corresponding to the case $`p=0`$. To be more precise, we pose the following question:

*Let $`\mathrm{\Omega }`$ and $`v`$ be as above. Let $`\gamma n`$ and let $`\psi :_+_+`$ be permissible. Does the condition*

$$_\mathrm{\Omega }\psi (|v(x)|)\delta (x)^\gamma 𝑑m(x)<\mathrm{},$$

*imply $`v0`$?*

Observe that the least severe form of above integrability condition occurs when $`\gamma =n`$.

Below in Corollary 4.5 we answer the question in the affirmative, in the case of any strictly permissible function $`\psi `$. In order to achieve this, we first formulate below in Theorem 4.3 a general result for arbitrary $`\gamma 2`$ which is, for $`n<\gamma 2`$, however, essentially more or less just Suzuki’s above result (see Remarks 4.4 (b) below). Our formulation has the advantage that, unlike Suzuki’s result, it contains a certain limiting case, Corollary 4.5, too.

The proof which we below write down (and in quite detail, just for the convenience of the reader) is merely a slight modification of Suzuki’s argument, combined with our version for the generalized mean value inequality (Theorem 2.5 above), and also some additional estimates.

4.2 Lemma. *Let $`u`$ be a nonnegative subharmonic function on $`\mathrm{\Omega }`$. Suppose $`\psi :_+_+`$ is a permissible function such that*

$$_\mathrm{\Omega }\psi (u(x))\delta (x)^\gamma 𝑑m(x)<\mathrm{}$$

*for some $`\gamma `$. Then $`\psi (u(x))=o(\delta (x)^{n\gamma })`$ as $`\delta (x)0`$.*

Proof. By Theorem 2.5, $`\psi u`$ is quasi-nearly subharmonic on $`\mathrm{\Omega }`$. Write for $`x\mathrm{\Omega }`$, $`B=B(x,\delta (x))`$ and $`B_0=B(x,\frac{\delta (x)}{2})`$. Since

(7)
$$\frac{1}{2}\delta (x)<\delta (y)<\frac{3}{2}\delta (x)$$

for all $`yB_0`$, we get

$$\begin{array}{cc}\hfill \psi (u(x))& 2^{n+|\gamma |}C_0\delta (x)^{n\gamma }_{B_0}\psi (u(y))\delta (y)^\gamma 𝑑m(y)\hfill \\ & C\delta (x)^{n\gamma }_{\mathrm{\Omega }_{\delta (x)}}\psi (u(y))\delta (y)^\gamma 𝑑m(y),\hfill \end{array}$$

where $`C=C(\gamma ,n,\psi ,u)>0`$ and $`\mathrm{\Omega }_{\delta (x)}=\{y\mathrm{\Omega }:\delta (y)<\delta (x)\}`$. The claim follows.  ∎

4.3 Theorem. *Let $`\mathrm{\Omega }`$ be bounded. Let $`v`$ be a superharmonic (resp. nonnegative subharmonic) function on $`\mathrm{\Omega }`$. Let $`\psi :_+_+`$ be a strictly permissible function. Suppose*

(8)
$$_\mathrm{\Omega }\psi (|v(x)|)\delta (x)^\gamma 𝑑m(x)<\mathrm{},$$

*where $`\gamma 2`$ is such that there is a constant $`C=C(\gamma ,n,\psi ,\mathrm{\Omega })>0`$ such that*

(9)
$$s^{n+\gamma }\psi (Cs^{n2})\text{ for all }s>\frac{1}{\text{diam}\mathrm{\Omega }}.$$

*Then $`v`$ vanishes identically.*

4.4 Remarks. Next we consider the assumptions in Theorem 4.3.

* Our assumption $`\gamma 2`$ is unnecessary, and it could be dropped: If $`\gamma `$, then it follows easily from $`(9)`$ and from the property (c) in 2.2 of strictly permissible functions that indeed $`\gamma 2`$.
* Suppose that $`n<\gamma 2`$. If, instead of $`(9)`$, one supposes that

$$s^{n+\gamma }\psi (Cs^{n2})\text{ for all }s>0,$$

then clearly

$$\psi (|v(x)|)C^{\frac{n+\gamma }{n2}}|v(x)|^{\frac{n+\gamma }{n2}}$$

for all $`x\mathrm{\Omega }`$. Thus $`(8)`$ implies that

$$_\mathrm{\Omega }|v(x)|^{\frac{n+\gamma }{n2}}\delta (x)^\gamma 𝑑m(x)<\mathrm{},$$

and hence $`v0`$ by Suzuki’s result, Theorem C above. Recall that here $`0<p=\frac{n+\gamma }{n2}1`$ and $`\gamma =npn2p`$. Thus Theorem 4.3, but now the assumption $`(9)`$ replaced with the aforesaid assumption, is just a restatement of Suzuki’s result for bounded domains.
* If $`\gamma n`$, then the condition $`(9)`$ clearly holds, since $`\psi `$ is strictly permissible. This case gives indeed the already referred limiting case for Suzuki’s result. See Corollary 4.5 below.

Proof of Theorem 4.3. We write the proof down only for the case $`n3`$. Write $`v^+=\mathrm{max}\{v,0\}`$ and $`s=v^{}=\mathrm{min}\{v,0\}`$. Then $`|v|=v^++v^{}`$ and $`s0`$ is subharmonic. (Resp. if $`v`$ is nonnegative and subharmonic, let $`s=v`$.) Proceeding as Suzuki, but using also some additional estimates, we will show that $`s0`$.

By $`(8)`$,

$$_\mathrm{\Omega }\psi (s(x))\delta (x)^\gamma 𝑑m(x)<\mathrm{},$$

thus

$$v_{\psi ,\gamma }(x)=_\mathrm{\Omega }G_\mathrm{\Omega }(x,y)\psi (s(y))\delta (y)^\gamma 𝑑m(y)<\mathrm{}$$

is a potential by \[Hel69, Theorem 6.3, p. 99\]. Here $`G_\mathrm{\Omega }`$ is the Green function of $`\mathrm{\Omega }`$.

By Lemma 4.2, $`\psi (s(y))C\delta (y)^{n\gamma }`$. Thus also

(10)
$$s(y)\psi ^1(C\delta (y)^{n\gamma })C\psi ^1(\delta (y)^{n\gamma })$$

for all $`y\mathrm{\Omega }`$, where $`C=C(\gamma ,n,\psi ,s,\mathrm{\Omega })1`$. Let $`x\mathrm{\Omega }`$ be fixed for a while. Let $`B=B(x,\delta (x))`$ and $`B_0=B(x,\frac{\delta (x)}{2})`$. Using $`(10)`$ (and $`(7)`$) one gets

$$s(y)C\psi ^1(\delta (y)^{n\gamma })C\psi ^1(2^{n+|\gamma |}\delta (x)^{n\gamma })C\psi ^1(\delta (x)^{n\gamma })$$

for all $`yB_0`$. Therefore

$$\frac{\psi (s(y))}{s(y)}C_1\frac{\psi (C\psi ^1(\delta (x)^{n\gamma }))}{C\psi ^1(\delta (x)^{n\gamma })}C\frac{\delta (x)^{n\gamma }}{\psi ^1(\delta (x)^{n\gamma })}$$

for all $`yB_0`$. With the aid of this and of a standard estimate for the Green function $`G_B(x,)`$ in $`B_0`$ and of $`(10)`$, one gets

$$\begin{array}{cc}\hfill v_{\psi ,\gamma }(x)& =_\mathrm{\Omega }G_\mathrm{\Omega }(x,y)\psi (s(y))\delta (y)^\gamma 𝑑m(y)_{B_0}G_B(x,y)\psi (s(y))\delta (y)^\gamma 𝑑m(y)\hfill \\ & _{B_0}G_B(x,y)s(y)\frac{\psi (s(y))}{s(y)}\delta (y)^\gamma 𝑑m(y)\hfill \\ & C\frac{\delta (x)^{n\gamma }}{\psi ^1(\delta (x)^{n\gamma })}_{B_0}|xy|^{2n}\delta (y)^\gamma s(y)𝑑m(y)\hfill \\ & C\frac{1}{\delta (x)^{n2}\psi ^1(\delta (x)^{n\gamma })}s(x).\hfill \end{array}$$

By $`(9)`$ we see that there is a constant $`C_31`$ such that

$$\delta (y)^{n2}\psi ^1(\delta (y)^{n\gamma })C_3$$

for all $`y\mathrm{\Omega }`$. Combining this with the above estimate for $`v_{\psi ,\gamma }`$, one gets

$$v_{\psi ,\gamma }(x)Cs(x),$$

where $`C=C(\gamma ,n,\psi ,s,\mathrm{\Omega })>0`$. Remembering that $`x\mathrm{\Omega }`$ was arbitrary, that $`v_{\psi ,\gamma }`$ is a potential and $`s`$ subharmonic, it follows from \[Hel69, Corollary 6.19, p. 117\] that $`s0`$. Thus $`v=v^+0`$. It remains to show that $`v0`$.

As above,

$$\begin{array}{cc}\hfill _\mathrm{\Omega }G_\mathrm{\Omega }(x,y)\delta (y)^2𝑑m(y)& _{B_0}G_B(x,y)\delta (y)^2𝑑m(y)\hfill \\ & C_{B_0}|xy|^{2n}\delta (y)^2𝑑m(y)\hfill \\ & C\delta (x)^{2n}\delta (x)^2\nu _n(\frac{\delta (x)}{2})^n=C,\hfill \end{array}$$

where $`C=C(n)>0`$. Thus by \[Hel69, Lemma 6.1, p. 98, and Corollary 6.19, p. 117\],

(11)
$$_\mathrm{\Omega }G_\mathrm{\Omega }(x,y)\delta (x)^2𝑑m(y)=\mathrm{}$$

for all $`x\mathrm{\Omega }`$. Consider next an arbitrary potential $`w`$ on $`\mathrm{\Omega }`$,

(12)
$$w(x)=_\mathrm{\Omega }G_\mathrm{\Omega }(x,y)𝑑\lambda (y)$$

where $`\lambda 0`$ is a measure on $`\mathrm{\Omega }`$. From $`(11)`$ it follows that

$$\begin{array}{cc}\hfill _\mathrm{\Omega }w(x)\delta (x)^2𝑑m(x)& =_\mathrm{\Omega }[_\mathrm{\Omega }G_\mathrm{\Omega }(x,y)𝑑\lambda (y)]\delta (x)^2𝑑m(x)\hfill \\ & =_\mathrm{\Omega }[_\mathrm{\Omega }G_\mathrm{\Omega }(x,y)\delta (x)^2𝑑m(x)]𝑑\lambda (y)=\mathrm{}.\hfill \end{array}$$

Using this and the facts that $`\mathrm{\Omega }`$ is bounded and $`w`$, as a superharmonic function, is locally integrable, one sees that

(13)
$$_{\mathrm{\Omega }_1}w(x)\delta (x)^2𝑑m(x)=\mathrm{}$$

where $`\mathrm{\Omega }_1=\{x\mathrm{\Omega }:\delta (x)<1\}.`$

Suppose in particular that $`w`$ in $`(12)`$ is the potential of the superharmonic function $`v_M=inf\{v,M\}`$, where $`M>0`$. Then $`v_Mw`$, and one has by $`(13)`$ and by the fact that $`\gamma 2`$,

$$\begin{array}{cc}\hfill \mathrm{}>_\mathrm{\Omega }\psi (v(x))\delta (x)^\gamma 𝑑m(x)& _\mathrm{\Omega }\psi (v_M(x))\delta (x)^\gamma 𝑑m(x)\hfill \\ & _\mathrm{\Omega }v_M(x)\frac{\psi (v_M(x))}{v_M(x)}\delta (x)^\gamma 𝑑m(x)\hfill \\ & C\frac{\psi (M)}{M}_\mathrm{\Omega }v_M(x)\delta (x)^\gamma 𝑑m(x)\hfill \\ & C\frac{\psi (M)}{M}_{\mathrm{\Omega }_1}w(x)\delta (x)^2𝑑m(x)=\mathrm{},\hfill \end{array}$$

a contradiction unless $`w0`$. Since $`w0`$, the nonnegative superharmonic functions $`v_M`$, $`M>0`$, are in fact harmonic, e.g. by the Riesz Decomposition Theorem \[Hel69, Theorem 6.18, p. 116\]. Since this is impossible, one has $`v0`$, concluding the proof.  ∎

4.5 Corollary. *Let $`\mathrm{\Omega }`$ be bounded. Let $`v`$ be a superharmonic (resp. nonnegative subharmonic) function on $`\mathrm{\Omega }`$. Let $`\psi :_+_+`$ be any strictly permissible function and let $`\gamma n`$. If*

$$_\mathrm{\Omega }\psi (|v(x)|)\delta (x)^\gamma 𝑑m(x)<\mathrm{},$$

*then $`v`$ vanishes identically.*

For the proof observe that the condition $`(9)`$ is indeed satisfied for $`\gamma n`$, since $`\mathrm{\Omega }`$ is bounded and $`\psi `$ is increasing.  ∎

4.6 Remark. The result of Theorem 4.3 does not, of course, hold any more, if one replaces strictly permissible functions by permissible functions. For a counterexample, set, say, $`v(x)=|x|^{2n}`$, $`\psi (t)=t^p`$, where $`\frac{n1}{n2}<p<\frac{n}{n2}`$, $`\gamma =npn2p`$ or just $`\gamma >1`$. Then clearly

$$_Bv(x)^p\delta (x)^\gamma 𝑑m(x)<\mathrm{}$$

but $`v0`$.

4.7 Remark. Provided $`\mathrm{\Omega }`$ is bounded and $`\psi `$ is strictly permissible, one can, with the aid of Theorem 4.3 and Corollary 4.5, exclude some trivial cases $`u0`$ from the result of Theorem 3.4 by imposing certain restrictions on the exponent $`\gamma `$. We point out only two cases:

* By Corollary 4.5, $`\gamma >n`$, regardless of $`\psi `$.
* By Suzuki’s result, Theorem C above, $`\gamma >npn2p`$, in the case when $`\psi (t)=t^p`$, $`0<p1`$.

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