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# Long lived acoustic vibrational modes of an embedded nanoparticle

## Abstract

Classical continuum elastic calculations show that the acoustic vibrational modes of an embedded nanoparticle can be lightly damped even when the longitudinal plane wave acoustic impedances $`Z_o=\rho v_L`$ of the nanoparticle and the matrix are the same. It is not necessary for the matrix to be less dense or softer than the nanoparticle in order to have long lived vibrational modes. A corrected formula for acoustic impedance is provided for the case of longitudinal spherical waves. Continuum boundary conditions do not always accurately reflect the microscropic nature of the interface between nanoparticle and matrix, and a multi-layer model of the interface reveals the possibility of additional reduction of mode damping.

A classical vibrational mode weakly coupled to a cold environment will have an amplitude exponentially decaying with time. The vibrational frequency of the mode may be slightly shifted from what it would have been if the environmental coupling is reduced to zero. When coupling is stronger, the mode loses its individual identity, and it becomes necessary instead to consider normal modes of the entire system.

Nearly spherical clusters of atoms a few nanometers in size (nanoparticles) have mechanical vibrations which can be initiated through sudden thermal excitation with a brief laser pulse.Voisin et al. (2001) Subsequent evolution of the vibration can be followed by observing the amount of light absorption by a probe pulse following the pump pulse by a controlled time.

It is rarely possible to perform such experiments on isolated nanoparticles. Normally there is mechanical coupling to an environment. This can be (1) a powder of nanoparticles (where adsorption is important) (2) a substrate to which the nanoparticle is attached (3) liquid solution or (4) a solid surrounding matrix, usually glass. Propagation of acoustic waves away from the nanoparticle is often the dominant mechanism for mechanical energy loss. As a result, vibrational modes are damped.

The organization of this paper is as follows: We begin with the current “state of the art” of vibration eigenmode calculation for free and matrix-embedded spheres. Then we focus on a particular material combination which gives rise to very low damping of the fundamental “breathing” mode even though the longitudinal plane wave acoustic impedances in the two materials are the same. We then derive the correct expression for the acoustic impedance for such modes and explain this result. Finally, we extend the calculation to more realistic materials where the sphere-matrix contact is not perfect and to modes having different symetries.

A quantum mechanical analysis of energy loss of a nanoparticle weakly coupled to a substrate heat bath has been done.Patton and Geller (2003) Otherwise, the nanoparticle has been approximated as a classical isotropic homogeneous linear elastic continuum object in contact with a similarly idealized zero temperature matrix. We consider such a spherical nanoparticle of radius $`R_p`$, density $`\rho _p`$ and speeds of sound $`v_{Lp}`$ and $`v_{Tp}`$ embedded within a macroscopic matrix of density $`\rho _m`$ and speeds of sound $`v_{Lm}`$ and $`v_{Tm}`$. Idealized continuum boundary conditionsBettenhausen et al. (2003) of continuous displacement and normal stress components have been applied where the nanoparticle contacts the matrix, but these will be reaxamined later on.

“Pseudomodes” of a nanoparticle embedded in a solid or fluid matrix can be foundDubrovskiy and Morochnik (1981) yielding complex valued frequencies $`\omega _{q\mathrm{}n}^{\mathrm{CFM}}`$ of the “complex frequency model” (CFM). $`q`$ can be torsional (TOR) or spheroidal (SPH). $`\mathrm{}`$ is the angular momentum and $`m`$ is the $`z`$-component. $`n0`$ is the mode index. $`Re(\omega _{q\mathrm{}n}^{\mathrm{CFM}})=2\pi /T`$ are shifted from $`\omega _{q\mathrm{}n}^{\mathrm{FSM}}`$ of a free sphere model (FSM) as first calculated in 1882 by LambLamb (1882) and some new modes appear.Murray and Saviot (2004) $`Im(\omega _{q\mathrm{}n}^{\mathrm{CFM}})=1/\tau =\frac{1}{2}\mathrm{\Delta }\omega `$ where $`\tau `$ is the damping time and $`\mathrm{\Delta }\omega `$ is the full width at half maximum (FWHM) of a Brillouin or Raman peak. The quality factor of each pseudomode is defined as $`Q=\omega /\mathrm{\Delta }\omega `$. This paper is mainly focused on (SPH,$`\mathrm{}=0`$) modes which are the only ones to have been experimentally observed in pump-probe experiments. These modes are also Raman active.

Interpretation of CFM is not straightforward, since the resulting pseudomodes are not orthonormalizable and blow up exponentially with the radial coordinate. This makes a correspondence to quantum theory unclear. An alternative is to calculate all of the normal modes of a nanoparticle (“core”) surrounded by a large spherical matrix (“shell”), imposing an arbitrary condition on the matrix outer surface.Portalès et al. (2002) The resulting core-shell model (CSM) is conservative and has real valued mode frequencies.Murray and Saviot (2004) However, there is a continuum of normal modes in the macroscopic limit that the matrix radius is infinite. Note that highly damped “matrix modes”Murray and Saviot (2004) are not considered in this work.

The connection between the continuum of CSM modes and the discrete spectra of CFM pseudomodes is clearly seen by making a plot of the mean squared displacement within the nanoparticle $`u^2_p`$ as a function of frequency for CSM modes.Murray and Saviot (2004) The resulting peaks correspond closely to $`Re(\omega _{q\mathrm{}n}^{\mathrm{CFM}})`$ and the FWHM of the CSM peaks corresponds closely to $`2Im(\omega _{q\mathrm{}n}^{\mathrm{CFM}})`$.

Even without applying the complexities of CFM or CSM, the qualitative effect of the matrix in shifting and broadening FSM frequencies can often be correctly anticipated by comparing the longitudinal plane wave acoustic impedances (LPWAI) $`Z_{op}=\rho _pv_{Lp}`$ and $`Z_{om}=\rho _mv_{Lm}`$.

The “rule of thumb” is that nanoparticle vibrational modes will be lightly damped when the LPWAI’s satisfy $`Z_{op}Z_{om}`$ or $`Z_{op}Z_{om}`$. Otherwise, similar LPWAI’s of the nanoparticle and matrix allow vibrational energy to freely flow out, resulting in strong damping.

Here we report dramatic exceptions to this. It is possible for a nanoparticle to have lightly damped normal modes without LPWAI’s $`Z_{om}`$ and $`Z_{op}`$ being very different, with the extreme possibility of $`\tau `$ being large even if $`Z_{om}=Z_{op}`$. Furthermore, lightly damped nanoparticle frequencies can differ greatly from $`\omega _{q\mathrm{}n}^{\mathrm{FSM}}`$. These possibilities have remained obscure up to now because experiments were limited primarily to situations in which the LPWAI’s satisfied $`Z_{op}>Z_{om}`$ for which FSM works extremely well. Furthermore, nanoparticle size variation within a sample creates extrinsic broadening of the modes which can sometimes exceed intrinsic broadening.

An example will illustrate when such unexpected results can occur: a gold nanoparticle embedded in a diamond matrix. We use the elastic constants of bulk fcc gold at 300 KHearmon (1984) and use directional averagingSaviot et al. (2004a) to obtain longitudinal and transverse speeds of sound of 3330 m/s and 1250 m/s respectively. We use elastic constants for bulk crystalline diamond at 300 KMcSkimin and Bond (1972) and similarly obtain speeds of sound 18190 m/s and 12350 m/s. The resulting LPWAI’s are identical: $`Z_{op}Z_{om}6.410^7\text{kg m}^2\text{s}^1`$. In the absence of any apparent impedance mismatch, the “rule of thumb” says that the vibrational modes of the nanoparticle would become so broadened by the presence of the matrix as to be unrecognizable.

Figure 1 shows something completely different. $`u^2_p`$ for CSM (SPH,$`\mathrm{}=0`$) modes is plotted versus frequency. For comparison, $`\omega _{q\mathrm{}n}^{\mathrm{CFM}}`$ are plotted showing $`Re(\omega )`$ as a vertical arrow with horizontal arrows to indicate $`Im(\omega )`$ which is half the FWHM. The resulting CSM peaks and $`Re(\omega _{q\mathrm{}n}^{\mathrm{CFM}})`$ match very closely. The gold nanoparticle has several lightly damped modes of vibration.

Figure 2 shows how misleading naive comparison of LPWAI’s can be. It was obtained by varying both $`\rho _m`$ and $`v_{Lm}`$ while keeping $`Z_{om}=Z_{op}`$. Mode broadening is large only when $`v_{Lm}<v_{Lp}`$. Note that for a gold nanoparticle in diamond, $`v_{Tm}/v_{Lm}0.68`$ and $`\rho _m/\rho _p0.18`$. For low matrix mass density, the frequency approaches that of the bound sphere model (BSM), $`\omega _{\mathrm{SPH00}}^{\mathrm{BSM}}`$, which is for a sphere with zero displacement boundary conditions.

For a purely longitudinal spherical wave in an isotropic elastic medium, the acoustic impedance is $`Z=\sigma _{rr}/v_r`$ where stress component $`\sigma _{rr}=2\rho v_T^2e_{rr}+\rho (v_L^22v_T^2)(e_{rr}+e_{\theta \theta }+e_{\varphi \varphi })`$ and velocity $`v_r=u_r/t`$. For this case strain $`e_{rr}=u_r/r`$ and $`e_{\theta \theta }=e_{\varphi \varphi }=u_r/r`$. The radial displacement is $`u_r=e^{i\omega t}(d/dr)(e^{ik_Lr}/r)`$ where $`\omega =v_Lk_L`$. The resulting expression for impedance is

$$Z(s)=\frac{\rho (v_L^2+4v_T^2(iss^2))}{v_L(1+is)}$$
(1)
where $`s=1/(k_Lr)`$. This can only be applied to the case of (SPH,$`\mathrm{}=0`$) modes. In the plane wave limit (large $`r`$) $`Z\rho v_L`$. For a fluid medium, $`v_T=0`$ so that $`Z=\rho v_L/(1+is)`$, a result familiar for sound wavesKinsler et al. (2000). Another interesting case is Poisson ratio $`\nu =\frac{1}{3}`$ (approximately true of many materials) where $`v_T=\frac{1}{2}v_L`$ so that $`Z=\rho v_L`$ to linear order in $`s`$. Note that $`v_T/v_L=\sqrt{\frac{12\nu }{22\nu }}`$.

If $`s`$ is small, then $`Re(Z)\rho v_L`$ and $`Im(Z)s\rho v_L(4(v_T/v_L)^21)`$. Note that if $`v_T=\frac{1}{2}v_L`$ then $`Im(Z)`$ is approximately zero.

Define $`\alpha =v_{Lm}/v_{Lp}`$. Let $`Z_p(1/\xi )`$ and $`Z_m(\alpha /\xi )`$ denote the acoustic impedance evaluated at $`R_p`$ of the nanoparticle and matrix respectively for outgoing waves of dimensionless frequency $`\xi =\omega R_p/v_{Lp}`$. Note that for a given pseudomode, these impedances do not depend on $`R_p`$. If $`Z_p(1/\xi )=Z_m(\alpha /\xi )`$ then a longitudinal travelling wave can cross the nanoparticle-matrix interface without any reflection.

Consider $`Z_p(1/\xi )`$: for the (SPH,$`\mathrm{}=0`$,$`n`$) FSM mode, $`s(r=R_p)\frac{1}{(n+1)\pi }`$. For the fundamental ($`n=0`$) mode $`s(r=R_p)`$ is not small and $`Z_p(1/\xi )`$ is complex-valued. But for higher order modes $`s`$ becomes small so that $`Z_p(1/\xi )\rho _pv_{Lp}`$. Thus, it is expected that the acoustic impedance mismatch at the nanoparticle-matrix interface will be different for higher order modes. Figure 1 confirms this. Also, as predicted in a previous paperMurray and Saviot (2004), the area under each pseudomode is roughly constant in the $`u^2_p`$ plot. This is important because it means that less damped modes compensate their lower frequency broadening with a higher mean square displacement and therefore can have similar electron-phonon coupling inside the nanoparticle as more damped modes.

Consider the longitudinal radial ($`r`$) velocity within the nanoparticle ($`p`$) to be the sum of inward ($`i`$) and outward ($`o`$) travelling waves:

$$v_{rpo}(x)=e^{i\omega t}A_{po}\omega e^{ix}((1/x)+(i/x^2))$$
(2)
$$v_{rpi}(y)=e^{i\omega t}A_{pi}\omega e^{iy}((1/y)+(i/y^2))$$
(3)
where $`x=\omega r/v_{Lp}`$ and $`y=\omega r/v_{Lp}`$. $`A_{po}`$ and $`A_{pi}`$ are amplitudes. To avoid singularity at the origin, $`A_{po}=A_{pi}`$. Matching of boundary conditions at the interface at $`R_p`$ corresponds to the equation:

$$\frac{Z_p(1/\xi )Z_m(\alpha /\xi )}{Z_p(1/\xi )+Z_m(\alpha /\xi )}=\frac{v_{rpi}(\xi )}{v_{rpo}(\xi )}$$
(4)
The roots of this equation are the complex valued dimensionless frequencies $`\xi _{\mathrm{SPH0}n}^{\mathrm{CFM}}`$. This equation is equivalent to previous solutionsDubrovskiy and Morochnik (1981) of CFM for the (SPH,0) case, but clearly illustrates the role of the acoustic impedances in determining the mode frequencies.

Previous studiesVoisin et al. (2002) were restricted to analyzing the situation of a soft, light matrix where $`v_{Lm}<v_{Lp}`$ and $`\rho _m<\rho _p`$, and found that $`\tau `$ does not depend on $`n`$. But we find that in other situations damping can vary dramatically with mode order, as clearly seen in Fig. 1.

In the matrix, $`s=\alpha /\xi `$ can be small if $`v_{Lm}v_{Lp}`$. But if $`v_{Lm}v_{Lp}`$ then $`s`$ can be large, and in this limit $`Z_m(\alpha /\xi )4i\rho _mv_{Tm}^2/(\omega R_p)`$, and the effect of the matrix is a purely restorative force, as if the matrix is a massless spring. Energy cannot be absorbed by the matrix in this limit, so that $`\tau \mathrm{}`$ when $`v_{Lp}/v_{Lm}0`$.

We have explored the lowest (SPH,$`\mathrm{}=0`$) mode (ignoring highly damped “matrix modes” when they are present) in the parameter space of $`\rho _p`$, $`\rho _m`$, $`v_{Lp}`$, $`v_{Tp}`$, $`v_{Lm}`$ and $`v_{Tm}`$ and found some general patterns. Notably, good impedance matching between nanoparticle and matrix as exhibited in very strong lowest (SPH,0) mode damping is an unusual occurence requiring special conditions. Closeness of the LPWAI’s alone is not sufficient.

If $`\nu _m\nu _p`$ (where $`\nu _m`$ and $`\nu _p`$ are the Poisson ratios of the matrix and particle respectively) then there is never strong damping, but we can have strong damping if $`\nu _m\nu _p`$ such as for a liquid matrix. Assuming the Poisson ratios are close, it is usually necessary that $`\rho _m\rho _p`$ and $`v_{Lm}v_{Lp}`$. Under these conditions, $`s`$ is small in the matrix and the LPWAI’s are close to the true impedances. In addition, if $`\nu _m`$ and $`\nu _p`$ are both close to $`\frac{1}{3}`$ then strong damping is still possible if $`\rho _m`$ is as little as $`0.8\rho _p`$. Conversely, light damping is always seen when any of the following conditions is satisfied: (1) $`\nu _p\nu _m`$ (2) $`\rho _m0.8\rho _p`$ (3) $`v_{Lm}1.2v_{Lp}`$.

As was shown in a previous work,Portalès et al. (2002) the microscopic details of the interface (e.g. the specific nature of the mechanical connection of the gold crystal lattice to the diamond matrix) can tend to isolate (i.e. decouple) the nanoparticle from the surrounding medium. In particular, continuum-type boundary conditions applied to the interface may not be optimal.Bettenhausen et al. (2003) One rough-and-ready way to adapt the CFM and CSM models to tentatively take this into account is to introduce an intermediate shell layer (X-layer) of inner radius $`R_pd_X/2`$, outer radius $`R_p+d_X/2`$, density $`\rho _X`$ and speeds of sound $`v_{LX}`$ and $`v_{TX}`$. Depending on the elaboration process, the nanoparticle and the surrounding matrix do not necessarily tightly adhere. Different expansion coefficients for example could result in a void in the matrix bigger than the nanoparticle and the nanoparticle being only partially in contact with the matrix. The X-layer is the most elementary way to explore the effect of deviations from continuum boundary conditions. Such calculations are relatively easy to perform using CFM or CSM.

It is important to demonstrate the robustness of CFM results against the microscopic details of the interface. The nature of the interface is unknown, but it can be guessed to be of lower density, poorly-ordered and not strongly-bonded. It is plausible to assume a low density and low elastic constants comparable to water or plastic. If $`d_X`$ is thin, neither $`\rho _X`$ nor $`v_{TX}`$ have a strong effect. What is important is the elastic constant of the X-layer in terms of $`\rho _Xv_{LX}^2`$ relative to the thickness of the X-layer, $`d_X`$. It is convenient to introduce the dimensionless parameter $`\sigma _X=d_X\rho _pv_{Lp}^2/(R_p\rho _Xv_{LX}^2)`$. For examples we looked at, the larger $`\sigma _X`$ is, the larger $`\tau `$ and $`Q`$ become.

A possible example of this may have been seen for gold nanoparticles embedded in TiO2. This is unrelated to our previous example of Au in diamond. Experimental observations of nanoparticle “breathing modes” (those with purely radial vibration) for Au nanoparticles in a TiO2 matrix using the femtosecond pump probe techniqueQian et al. (2000) reveal surprisingly light damping. Qian et al. obtained an oscillation frequency of 0.15 THz (5 cm-1) with a damping time of 55 ps ($`Q26`$) for $`R_p=10`$ nm. We use TiO2 sound speeds of 8610 m/s and 5160 m/s and density 4.097 g/cm3.Minnear and Bradt (1977) Our XCFM calculations for very small $`\sigma _X`$ predict $`\tau (10.7+21.0\sigma _X)`$ ps or $`Q5.92+11.7\sigma _X`$. This $`\tau `$ provides only an upper bound on the experimental damping time because of dephasing due to particle size variation. The large $`\tau `$ of Au in TiO2 could be obtained by a water-like layer between the nanoparticle and the matrix on the order of 0.1 nm thick. Thus, details of the nanoparticle-matrix interface at the atomic level are crucial in determining the damping of embedded nanoparticle vibrational modes. However, proper first-principles quantitative modelling of the interface requires consideration of detailed features of crystal and electronic properties at the atomic level, in particular the nature of the bonding.Carrier et al. (2002) For the systems we consider, there is insufficient information about the interface to attempt such a calculation, especially since the matrix is amorphous.

The ability to choose the matrix so as to have nanoparticles with lightly damped vibrational modes is important for several reasons. First, by reducing homogeneous broadening, it allows inhomogeneous broadening effects to stand out clearly. This results in a clearer picture for femtosecond pump-probe experiments where the damping time is longer but also in low frequency Raman experiments where a better separation of scattering lines is possible. Second, as was shown by the pump-pump-probe experiments in Del Fatti et al.Del Fatti et al. (2000) it is possible to control the acoustic motion of silver nanoparticles. With higher $`Q`$ factor, the first pump pulse would “launch” the motion of every nanoparticles but the next pump pulse could selectively enhanced the vibration amplitude of a smaller subset of the nanoparticles.

Solid matrix-embedded nanoparticles always have $`Q`$ factor lower than free ones. However, free nanoparticles suffer from many drawbacks. For example, surface adsorption can affect their properties. Also it is often technologically easier to deal with matrix embedded nanoparticles. Where solid embedding is technologically desirable, our results provide guidance about how the matrix can be optimally chosen.

Finally, the sphere radius is irrelevant in this paper ($`Q`$ does not depend on $`R`$). So there are some potential applications for other kinds of systems. Such damped vibrational modes of a virus in water may be relevant to its mechanical response to ultrasound.Saviot et al. (2004b)

All of the foregoing discussion applies only to spheroidal vibrations with $`\mathrm{}=0`$. A similar analysis can be carried out for torsional modes, but a separate expression for acoustic impedance is required for each value of $`\mathrm{}`$. It is not apparent how to make the extension to spheroidal modes with $`\mathrm{}0`$. Calculations made on CdS spheres embedded in silica in a previous workMurray and Saviot (2004) revealed lightly damped fundamental torsional modes which we could not understand at that time. The situation is even more dramatic for gold spheres inside diamond for which the lowest torsional modes have very high quality factors ($`Q900`$ for (TOR,$`\mathrm{}=1`$,$`n=0`$), $`Q20000`$ for (TOR,$`\mathrm{}=2`$,$`n=0`$), …)


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# Measurement of the Ξ⁰→Λ𝛾 Decay Asymmetry and Branching Fraction

## 2 Introduction

The $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ decay asymmetry plays an important role in solving a long standing discrepancy between the Hara theorem  and the observed decay asymmetries of weak radiative hyperon decays . The Hara theorem states that the parity-violating amplitude of weak radiative hyperon decays vanishes in the SU(3) limit. Accordingly, the decay asymmetries will vanish in this case. Introducing weak breaking of SU(3) symmetry one expects to observe small decay asymmetries. In contrast to this, a large negative decay asymmetry in the weak radiative decay $`\mathrm{\Sigma }^+p\gamma `$ was first measured by Gershwin et al.  and later confirmed . To address this observation, models were developed which tried to obtain large decay asymmetries in spite of weak SU(3) breaking. One category consists of pole models, which satisfy the Hara theorem by construction, and approaches based on chiral perturbation theory. They predict negative decay asymmetries for all weak radiative hyperon decays . Vector meson dominance models and calculations based on the quark model on the other hand violate the Hara theorem. It has been shown that the Hara theorem is generally violated in quark model approaches . This second group of models favours a positive decay asymmetry for the channel $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ . Therefore, the decay $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ plays a crucial role in differentiating between the groups of models. The only previous measurement of the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ decay asymmetry has been performed at FNAL, giving a value of $`0.43\pm 0.44`$ 111 The original publication  quoted a wrong sign of the asymmetry. This has been corrected in an erratum in 2002, but not yet in the PDG value ., and is not able to make the distinction.

In addition to the decay asymmetry, the branching fractions of radiative $`\mathrm{\Xi }^0`$ decays are similarly difficult to calculate. Predictions on the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ decay rate vary by about one order of magnitude . Two experiments have reported a branching fraction measurement , with the measured values being about two standard deviations apart. The latter measurement is an earlier NA48 measurement based on a data set of the year 1997, which contained only 31 $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ candidates.

In this letter we report a new measurement with greatly enhanced precision on both the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ decay asymmetry and branching fraction.

## 3 Experimental setup

The NA48 experiment has been designed for the measurement of direct CP violation in the decay of neutral kaons. However, due to the comparable life times, decays from $`\mathrm{\Lambda }`$ and $`\mathrm{\Xi }^0`$ hyperons could also be recorded by the NA48 detector. The experiment featured two almost collinear beams of neutral kaons which were derived from 450 GeV/$`c`$ protons hitting two fixed beryllium targets of 40 cm length and 0.2 cm diameter, which were located 6 m (near target) and 126 m (far target), respectively, upstream of the decay region . The present measurement is based on data from a special two-day run period in 1999 where only the near target was in operation. The proton beam was extracted from the CERN SPS in a 2.4 s spill every 14.4 s with the intensity increased to about $`5\times 10^9`$ protons per spill, which is a factor of $`200`$ higher than in normal running conditions. The near target was located 7.2 cm above the primary proton beam axis, which points to the detector centre. It was followed by a sweeping magnet with tungsten-alloy inserts in which the protons not interacting in the target were absorbed. The neutral beam was defined by a 0.36 cm diameter collimator 480 cm downstream of the target. It had a production angle of 4.2 mrad and a downward inclination of 0.6 mrad with respect to the incident proton beam, in order to have the axis of the neutral beam pointing to the centre of the electromagnetic calorimeter. The decay region was contained in an evacuated 89 m long and 2.4 m diameter steel tank, closed by a $`0.3\%`$ radiation lengths thick polyamide (Kevlar) composite window, from the centre of which a beam pipe traverses the following main NA48 detector.

The main NA48 detector elements are a magnetic spectrometer and a liquid-krypton electromagnetic calorimeter. The spectrometer is composed of two drift chambers  upstream and two downstream of a dipole magnet. The magnetic field is directed vertically and produces a 265 MeV/$`c`$ transverse momentum kick. The chambers provide 100 $`\mu `$m spatial resolution on the track coordinates, resulting in a total momentum resolution of $`\sigma (p)/p=0.6\%`$ for 45 GeV/$`c`$ particles.

The liquid-krypton calorimeter (LKr) measures the energies, positions, and times of electromagnetic showers initiated by photons and electrons. Around 20 t of liquid krypton at 121 K are used in a ionization detector. The calorimeter has a structure of 13212 square read-out cells of $`2\times 2`$ cm2 cross-section and 127 cm length (27 radiation lengths) each. The cross-section of the active volume has an octagonal shape of 240 cm inscribed diameter. The read-out cells are formed by longitudinally stretched copper-beryllium ribbons which act as electrodes. The energy resolution of the calorimeter is $`\sigma (E)/E=9\%/E3.2\%/\sqrt{E}0.42\%`$ with $`E`$ in GeV; the time resolution is better than 300 ps for photon energies above 20 GeV.

Further detector elements were used in the trigger decision for the present measurement: a steel-scintillator sandwich calorimeter (HAC) with a length of 6.7 nuclear interaction lengths follows the liquid-krypton calorimeter and measures energies and horizontal and vertical positions of hadron showers; a hodoscope composed of 64 horizontal and 64 vertical scintillator strips is located about 1.6 m upstream of the LKr calorimeter. A more detailed description of the experimental set-up can be found elsewhere .

The trigger decision for neutral hyperon decays was based on information from the detector elements described above. A positive pre-trigger decision required at least one coincidence between a vertical and a horizontal hodoscope scintillator strip, a two track signature in the drift chambers, and the sum of the energies deposited in the electromagnetic and the hadron calorimeter larger than 35 GeV. The next trigger level used information from a preliminary track reconstruction: In order to reject $`K_S\pi ^+\pi ^{}`$ background events, a mass cut around the kaon mass for the $`\pi ^+\pi ^{}`$ hypothesis and a cut on the ratio $`p_+/p_{}`$ between the positive and negative track momenta were applied. This ratio is large for $`\mathrm{\Lambda }p\pi ^{}`$ decays where the proton carries the major fraction of the initial momentum, as opposed to background kaon decays where the two charged particles typically have a much lower momentum ratio. The trigger rejected a window with $`1/5<p_+/p_{}<5`$ ($`1/4`$ and 4 for a brief period at the start of the run) and $`|m_{\pi ^+\pi ^{}}m_K|<30`$ MeV/c2 (25 MeV/c2), where $`m_K`$ is the nominal kaon mass. Because of the high rate the triggered events were down-scaled with different factors between 4 and 8 during the two-day run period. The plot of $`m_{\pi ^+\pi ^{}}`$ versus $`p_+/p_{}`$ for the accepted events is shown in Fig. 1. In total, approximately 150 million triggers were collected, out of which 18 million events contained $`\mathrm{\Lambda }`$ hyperons.

The events were selected by a trigger optimised to select hadronic events for which the accuracy of the electromagnetic calorimeter information was not necessary. For this trigger, showers from the LKr were read-out only if their seed energy exceeded 1 GeV instead of the usual 100 MeV. Therefore a cluster energy correction was applied, which was determined from the reconstructed invariant $`\pi ^0`$ mass in $`K_L\pi ^+\pi ^{}\pi ^0`$ events from the same data sample. The correction was energy-dependent and ranged between $`3\%`$ and $`0.5\%`$ for photon energies between 5 and 20 GeV.

A Monte Carlo simulation based on GEANT 3.21  for the LKr calorimeter and a fast track simulation was used throughout this analysis. Special care was taken to adjust beam, target, and collimator geometries and positions to the data.

## 4 Method of the Asymmetry Measurement

For the asymmetry measurement we exploit the well-known decay asymmetry of the $`\mathrm{\Lambda }p\pi ^{}`$ decay. The $`\mathrm{\Lambda }`$ hyperons are longitudinally polarized by the parent process $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ with a polarization of $`\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )`$ in their rest frame. Effectively, one measures the distribution of the angle $`\mathrm{\Theta }_\mathrm{\Lambda }`$ between the incoming $`\mathrm{\Xi }^0`$ (corresponding to the outgoing $`\mathrm{\Lambda }`$ direction in the $`\mathrm{\Xi }^0`$ rest frame) and the outgoing proton in the $`\mathrm{\Lambda }`$ rest frame (see Figure 2):

$$\frac{dN}{d\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }}=N_0\left(1\alpha (\mathrm{\Lambda }p\pi ^{})\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }\right)$$

In this way the $`\mathrm{\Lambda }`$ is polarized by the $`\mathrm{\Xi }^0`$ decay and analysed by its own decay into $`p\pi ^{}`$. The minus sign is purely conventional and arises from the fact that the photon carries spin 1, which leads to an opposite $`\mathrm{\Lambda }`$ spin to that in the process $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ .

For calibration purposes and as a cross-check, we have also analyzed the decay $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$, for which the decay asymmetry is well measured. Obviously, when replacing $`\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )`$ with $`\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0)`$, there is no difference in the topology for the decays $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ and $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ and the definition of the angle $`\mathrm{\Theta }_\mathrm{\Lambda }`$ is similar. However, as explained above, the spin 0 nature of the $`\pi ^0`$ leads to a sign flip for the longitudinal $`\mathrm{\Lambda }`$ polarization.

## 5 Event Selection

The $`\mathrm{\Lambda }`$ hyperons were identified by two oppositely charged tracks in the spectrometer. The tracks were required to be at most 4.5 ns apart in time and to have momenta of at least 30 GeV/$`c`$ for the positive and 5 GeV/$`c`$ for the negative track. For both tracks the radial distances to the beam axis at the longitudinal positions of the drift chambers had to be greater than 12.6 cm to ensure full efficiency of the chambers. The extrapolation of the two tracks to the point of closest approach defined the $`\mathrm{\Lambda }`$ decay vertex. The distance of closest approach had to be less than 2.2 cm. The reconstructed $`\mathrm{\Lambda }`$ hyperon was required to have a minimum momentum of 57 GeV/$`c`$ and a reconstructed invariant mass within 2.7 MeV/$`c^2`$ of the nominal $`\mathrm{\Lambda }`$ mass, corresponding to a window of $`\pm 3`$ standard deviations. Finally, the longitudinal position of the $`\mathrm{\Lambda }`$ decay vertex had to be at least 6 m downstream of the target, corresponding to the end of the final collimator, and at most 40 m from the target.

Photons were detected by clusters in the electromagnetic calorimeter. The cluster energy had to be above 15 GeV. To ensure negligible energy loss, all clusters had to be at least 15 cm and at most 120 cm from the beam axis, well within the sensitive volume of the LKr calorimeter, and had to have a distance greater than 2 cm to any dead calorimeter cell. To avoid effects from hadron shower contaminations, the photon clusters were required to be separated by at least 25 cm from the impact point of any track. The cluster-time had to be within $`\pm 3`$ ns of the average of the track times.

The energy centre-of-gravity at the longitudinal position of the calorimeter was defined as

$$\stackrel{}{r}_{cog}=\underset{i}{}\stackrel{}{r}_iE_i/\underset{i}{}E_i,$$

with the sums running over tracks and photon clusters. The positions $`\stackrel{}{r}_i`$ are either the cluster positions in case of photons or the coordinates of the tracks extrapolated from before the spectrometer to the LKr calorimeter. The energies $`E_i`$ are the photon cluster energies or are derived from the track momenta using the nominal particle masses. To avoid missing energy in the event, the position of the energy centre-of-gravity was required to be less than 7 cm from the detector axis. The target position and the energy centre-of-gravity $`\stackrel{}{r}_{cog}`$ defined the reconstructed line-of-flight of the $`\mathrm{\Xi }^0`$. The distance of the $`\mathrm{\Lambda }`$ decay vertex from the $`\mathrm{\Xi }^0`$ line-of-flight had to be less than 2 cm to ensure a well-reconstructed event. The $`\mathrm{\Xi }^0`$ decay vertex was reconstructed as the point of closest approach between the $`\mathrm{\Xi }^0`$ line-of-flight and and the $`\mathrm{\Lambda }`$ line-of-flight, which was determined from the reconstructed $`\mathrm{\Lambda }`$ decay vertex and 3-momentum. The longitudinal position of the $`\mathrm{\Xi }^0`$ decay vertex was required to be at least 5 m downstream of the target, 1 m before the end of the final collimator.

Background from $`K_S\pi ^+\pi ^{}\gamma `$ decays was completely discarded by rejecting all events with an invariant mass, under a $`\pi ^+\pi ^{}\gamma `$ hypothesis, within $`7.5`$ MeV/$`c^2`$ of the nominal kaon mass (corresponding to $`2.5`$ standard deviations of the resolution). Additional background comes from $`K_L\pi ^+\pi ^{}\pi ^0`$ decays as well as from time overlap of two events or hadronic interactions in the collimator region. Both accidental and hadronic background contain a real $`\mathrm{\Lambda }`$ decay together with one or two photons from a $`\pi ^0`$ decay. In order to reject this background together with $`K_L\pi ^+\pi ^{}\pi ^0`$ decays, we rejected all events which had one or more additional LKr calorimeter cluster within 5 ns of the average track-time and more than 25 cm from the track impact points in the calorimeter. Decays of $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ with one lost photon are strongly suppressed by kinematics to enter the signal region, even if resolution effects are taken into account.

The $`\mathrm{\Lambda }\gamma `$ invariant mass distribution of the $`\mathrm{\Xi }^0`$ candidates is shown in Figure 3. Within $`\pm 7.8`$ MeV/$`c^2`$ (3 standard deviations) of the $`\mathrm{\Xi }^0`$ mass 730 $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ candidates were reconstructed. As all remaining background sources have a flat distribution in a close invariant $`\mathrm{\Lambda }\gamma `$ mass interval, as seen from Monte Carlo simulation, we have used mass side-bands from $`1.3`$ to $`1.305`$ GeV/$`c^2`$ and from $`1.325`$ to $`1.335`$ GeV/$`c^2`$ for background subtraction. From this, the background was estimated to be $`58.2\pm 7.8`$ events, which corresponds to $`(8.0\pm 1.1)\%`$ of the signal sample. It is dominated by hadronic events with some remaining contributions from accidental background and mis-identified $`K_L\pi ^+\pi ^{}\pi ^0`$ decays.

For the selection of the normalization channel $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ only a few changes were applied with respect to the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ selection. At least two photon clusters within 5 ns and with energies above 6 GeV were required. The invariant mass of the two photons, computed using the cluster energies and positions and the reconstructed $`\mathrm{\Xi }^0`$ decay vertex, had to be within 3 standard deviations (about 10 MeV/$`c^2`$) from the nominal $`\pi ^0`$ mass. No cut on additional LKr calorimeter clusters was applied for the $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ selection.

After applying all selection criteria, the total yield of $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ candidates was 61828 events within a window of $`\pm 3.0`$ MeV/$`c^2`$ ($`3\sigma `$) around the nominal $`\mathrm{\Xi }^0`$ mass (Fig. 4). Backgrounds are negligible in this channel.

## 6 Measurement of the Decay Asymmetry

As described, the asymmetry is analysed in the angle $`\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }`$. The resolution on $`\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }`$ is 0.01, as determined from the Monte Carlo simulation. Fig. 5a shows the $`\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }`$ distributions for all $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ candidates and for the properly scaled side-band events compared to the isotropic Monte Carlo simulation.

The ratio of data over Monte Carlo corrects for the detector acceptance. To account for the background contamination, an effective asymmetry $`\alpha _{\text{bkg}}`$ of the background was determined by fitting the side-band events with $`dN/d\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }1\alpha _{\text{bkg}}\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }`$. The result of $`\alpha _{\text{bkg}}=0.13\pm 0.32`$ (together with the background fraction of $`(8.0\pm 1.1)\%`$) was used to apply a smooth correction to the $`\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }`$ distribution of the signal events for the background contamination. The ratio of background-corrected signal over Monte Carlo is shown in Figure 5b. A fit with the normalization and the asymmetry $`\alpha (\mathrm{\Lambda }p\pi ^{})\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )`$ as free parameters was performed in the range $`0.8<\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }<1`$, where both data and Monte Carlo statistics are large. The result of the fit is $`\alpha (\mathrm{\Lambda }p\pi ^{})\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )=0.50\pm 0.12_{\text{stat}}`$ with a $`\chi ^2`$ per degree of freedom of $`9.4/7`$. After dividing by $`\alpha (\mathrm{\Lambda }p\pi ^{})=0.642\pm 0.013`$  we obtain $`\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )=0.78\pm 0.18_{\text{stat}}`$.

Several contributions to the systematic error have been studied. The largest uncertainties come from the effective asymmetry of the background ($`\pm 0.052`$) and the background normalization ($`\pm 0.019`$). Additional uncertainties may arise from a possible incorrect modeling of the detector acceptance. This was investigated with $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ events, which have sufficient statistics, and which are, due to the lower $`Q`$ value, more sensitive to possible inefficiencies near the beam pipe. Different geometrical acceptance cuts in the beam pipe regions and on the $`\mathrm{\Xi }^0`$ energy as well as uncertainties in the beam profile simulation and the $`p_T`$ distribution of the $`\mathrm{\Lambda }`$ hyperons have been studied, resulting in a variation of $`\pm 0.007`$ on the decay asymmetry. The effect of transverse $`\mathrm{\Xi }^0`$ polarization on the decay asymmetry was studied and found to be negligible compared to the other uncertainties. Finally, the uncertainty on the used value of $`\alpha (\mathrm{\Lambda }p\pi ^{})`$ contributes $`\pm 0.016`$ to the systematics.

By adding the single components in quadrature, the total systematic uncertainty is $`\pm 0.06`$, which is small compared to the statistical uncertainty of the data (Tab. 1).

An important check for the validity of the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ analysis is the measurement of the decay asymmetry in $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$, where the data statistics is a factor of 100 higher. Both channels are two-body decays and the decay $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$, due to the lower $`Q`$ value, is even more sensitive to effects from the beam-line geometry and polarization than $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$. The decays $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ were recorded with the same trigger, analysed with the same definition of $`\mathrm{cos}\mathrm{\Theta }_\mathrm{\Lambda }`$, and used a similar Monte Carlo simulation as for the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ analysis. From our data we measure a combined $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ asymmetry of $`\alpha (\mathrm{\Lambda }p\pi ^{})\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0)=0.257\pm 0.011_{\text{stat}}`$. The excellent agreement between this result and the best published measurement of $`\alpha (\mathrm{\Lambda }p\pi ^{})\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0)=0.260\pm 0.006`$  validates the method and serves as a systematic check.

As a further check, a second analysis, which was performed using the same data but different Monte Carlo samples, gave consistent results.

## 7 Measurement of the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ Branching Fraction

Using the central value of our new result on the decay asymmetry, the overall $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ reconstruction efficiency was determined to be $`5.4\%`$ from Monte Carlo simulation. For the normalization channel $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ the reconstruction efficiency was determined to be $`0.58\%`$. It is significantly lower than for the signal channel, as the proton receives less transverse momentum and escapes more often undetected through the beam-pipe. Subtracting the background and using $`\mathrm{Br}(\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0)=99.5\%`$ , we obtain $`\mathrm{Br}(\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )=(1.16\pm 0.05_{\text{stat}})\times 10^3`$.

The systematic error is dominated by the uncertainty on the decay asymmetry, which leads to a $`\pm 4.8\%`$ uncertainty on the geometrical acceptance and therefore on the branching ratio. Other systematic uncertainties are the detector acceptance ($`\pm 1.1\%`$ of the measured value), the $`\mathrm{\Xi }^0`$ polarization ($`\pm 1.4\%`$), and the background estimation ($`\pm 1.1\%`$), which have been determined in a similar way to those for the decay asymmetry measurement. To account for the unknown $`\mathrm{\Xi }^0`$ polarization in our data we have varied the polarization in the simulation by $`\pm 10\%`$, which is similar in magnitude to the measured transverse $`\mathrm{\Xi }^0`$ polarization of about $`10\%`$ for a proton beam energy of 800 GeV and a production angle of 4.8 mrad . This variation resulted in a $`\pm 1.4\%`$ change of the measured branching fraction. An additional external uncertainty arises from the knowledge of the $`\mathrm{\Xi }^0\mathrm{\Lambda }\pi ^0`$ decay asymmetry ($`\pm 0.5\%`$), since it affects the selection efficiency of the normalization channel. Finally, the statistics of the normalization channel and of the signal and normalization Monte Carlo simulations contribute $`\pm 0.7\%`$ to the systematic uncertainty. All other sources of systematic errors were found to be negligible. The total systematic uncertainty on $`\mathrm{Br}(\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )`$ is $`\pm 5.3\%`$. A summary of uncertainties on the branching ratio measurement is given in Table 2.

A second independent analysis has been performed also for the branching fraction measurement and yielded a consistent result.

## 8 Summary and Conclusion

From the data of two days of high intensity $`K_S`$ data taking of the NA48 experiment 730 $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ candidates have been found with an estimated background of $`58.2\pm 7.8`$ events. By comparison with an isotropic Monte Carlo simulation, the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ decay asymmetry has been found to be

$$\alpha (\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )=0.78\pm 0.18_{\text{stat}}\pm 0.06_{\text{syst}}.$$

This is the first evidence for a negative decay asymmetry in this channel . As has been indicated in the introduction, the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ decay asymmetry is a crucial input parameter for theoretical approaches to weak radiative hyperon decays. The negative sign of the asymmetry clearly prefers models consistent with the Hara theorem, while, on the other hand, it cannot be easily explained by quark models and models using vector meson dominance.

In addition we have determined the $`\mathrm{\Xi }^0\mathrm{\Lambda }\gamma `$ branching fraction to

$$\mathrm{Br}(\mathrm{\Xi }^0\mathrm{\Lambda }\gamma )=(1.16\pm 0.05_{\text{stat}}\pm 0.06_{\text{syst}})\times 10^3,$$

which is the most precise measurement of this decay rate so far. It confirms the previous FNAL measurement , while being about 1.9 standard deviations below the previous NA48 measurement .

## 9 Acknowledgements

It is a pleasure to thank the technical staff of the participating laboratories, universities, and affiliated computing centres for their efforts in the construction of the NA48 apparatus, in the operation of the experiment, and in the processing of the data. We also would like to thank Piotr Żenczykowski for many useful discussions and insights into the theoretical interpretation of the result.


text:
# Light-ion production in the interaction of 96 MeV neutrons with silicon

## Abstract

Double-differential cross sections for light-ion (p, d, t, 3He and $`\alpha `$) production in silicon, induced by 96 MeV neutrons are reported. Energy spectra are measured at eight laboratory angles from $`20^{}`$ to $`160^{}`$ in steps of $`20^{}`$. Procedures for data taking and data reduction are presented. Deduced energy-differential, angle-differential and production cross sections are reported. Experimental cross sections are compared to theoretical reaction model calculations and experimental data in the literature.
PACS numbers: 25.40.-h, 25.40.Hs, 25.40.Kv, 28.20.-v

## 1 Introduction

In the last years, there has been an increasing request for experimental studies of fast-neutron induced reactions, especially at higher incident neutron energies. For basic physics, nucleon-induced reactions provide useful means to investigate nuclear structure, to characterize reaction mechanisms and to impose stringent constraints on nuclear model calculations. The silicon nucleus is sufficiently heavy for many of the statistical assumptions to hold (high density of excited states), yet not so heavy to give a strong suppression of charged particle emission due to Coulomb barrier effects. Therefore, nuclear reaction models for equilibrium and pre- equilibrium decay can be tested and benchmarked. Experimental data in the literature at incident neutron energies from reaction thresholds up to 60 MeV  and between 25 and 65 MeV  offer possibilities to test the predictions of reaction models.

In recent years, an increasing number of applications involving fast neutrons have been developed or are under consideration, e.g., radiation treatment of cancer , soft-error effects in computer memories , accelerator-driven transmutation of nuclear waste and energy production , and determination of the response of neutron detectors . Silicon data are particularly important for detailed soft-error simulation in electronic devices .

In this paper, we present experimental double-differential cross sections (inclusive yields) for protons, deuterons, tritons, 3He and alpha particles produced by 96 MeV neutrons incident on silicon. Measurements have been performed at the cyclotron of The Svedberg Laboratory (TSL), Uppsala, using the dedicated MEDLEY experimental setup . Spectra have been measured at 8 laboratory angles, ranging from $`20^{}`$ to $`160^{}`$ in $`20^{}`$ steps. Extrapolation procedures are used to obtain coverage of the full angular distribution and consequently energy-differential and production cross sections are deduced, the latter by integrating over energy and angle. The experimental data are compared to results of calculations with nuclear reaction codes and to existing experimental data.

The experimental methods are briefly discussed in sect. 2 and data reduction and correction procedures are presented in sect. 3 and 4, respectively. The theoretical framework is presented in sect. 5. In sect. 6, experimental results are reported and compared with theoretical and previous experimental data. Conclusions and an outlook are given in sect. 7.

## 2 Experimental setup and methods

The neutron beam facility at TSL uses the 7Li(p,n)7Be reaction (Q $`=1.64`$ MeV) to produce a quasi-monoenergetic neutron beam . The lithium target was 26 mm in diameter and 8 mm thick in the present experiment and enriched to 99.98 % in 7Li. The 98.5$`\pm `$0.3 MeV protons from the cyclotron impinge on the lithium target, producing a full-energy peak of neutrons at 95.6$`\pm `$0.5 MeV with a width of 1.6 MeV (FWHM) and containing 40 % of the neutrons, and an almost constant low-energy tail containing 60 % of the neutrons. The neutron beam is shaped by a collimator system, and delivered to the experimental area. After passage of the target, the proton beam is deflected by two magnets into a well-shielded beam dump, where the beam current is integrated in a Faraday cup. The integrated charge serves as one neutron beam monitor. With a beam intensity of about 5 $`\mu `$A, the neutron flux at the target location is about 5$``$104 neutrons/(s$``$cm2). The collimated neutron beam has a diameter of 80 mm at the location of the target. A thin film breakdown counter (TFBC)  installed after the reaction chamber is used as another beam monitor. The two beam monitor readings were in agreement during the measurements.

The charged particles are detected by the MEDLEY setup . It consists of eight three-element telescopes mounted inside a 100 cm diameter evacuated reaction chamber. Each telescope consists of two fully depleted $`\mathrm{\Delta }E`$ silicon surface barrier detectors and a CsI(Tl) crystal. The thickness of the first $`\mathrm{\Delta }E`$ detector ($`\mathrm{\Delta }E_1`$) is either 50 or 60 $`\mu `$m, while the second one ($`\mathrm{\Delta }E_2`$) is either 400 or 500 $`\mu `$m. They are all 23.9 mm in diameter (nominal). The cylindrical CsI(Tl) crystal, 50 mm long and 40 mm in diameter, serves as the $`E`$ detector. The back-end part of the crystal, 20 mm long, has a conical shape, tapered off to 18 mm diameter, to fit the size of a read-out diode.

To obtain a well-defined acceptance, a plastic scintillator collimator is placed in front of each telescope. The active collimators have an opening of 19 mm diameter and a thickness of 1 mm.

A Passivated Implanted Planar Silicon (PIPS) detector is used as an active target. It has a 32$``$32 mm2 quadratic shape and a thickness of 303 $`\mu `$m. It is suspended in a thin aluminium frame using threads and small springs. The dimensions of the frame have been chosen in such a way that it does not interfere with the incident neutron beam. Besides the energy deposited by the detected light ion, the active target recorded the energy deposition due to other products, like recoils, of the same event. This information was, however, not used in the present analysis.

For absolute cross section normalization, a 25 mm diameter and 1.0 mm thick polyethylene (CH2)n target is used. The $`np`$ cross section at $`20^{}`$ laboratory angle provides the reference cross section .

Background is measured by removing the target from the neutron beam. It is dominated by protons produced by neutron beam interaction with the beam tube and reaction chamber material, especially at the entrance and exit of the reaction chamber and in the telescope housings. Therefore, the telescopes at $`20^{}`$ and $`160^{}`$ are most affected. Since the protons in the background originated not from the target but came from different directions, they can be misidentified leading to a large background even for the other particles. For the $`160^{}`$ telescope, i.e., the worst case, the signal-to-background ratios are 2.5, 1 and 0.1 for protons, deuterons and tritons, respectively, whereas the corresponding numbers for the $`40^{}`$ telescope, i.e., the best case, are 8, 12 and 5. In the case of 3He and alpha particles, the background is negligible.

The time-of-flight (TOF) obtained from the radio frequency of the cyclotron (stop signal for the TDC) and the timing signal from each of the eight telescopes (start signal), is measured for each charged-particle event.

The raw data are stored event by event for on-line monitoring and subsequent off-line analysis. Typical count rates for target-in and target-out runs were 10 and 2 Hz, respectively. The dead time of the system was typically 1-2 % and never exceeding 10 %.

## 3 Data reduction procedures

### 3.1 Particle identification and energy calibration

The $`\mathrm{\Delta }EE`$ technique is used to identify light charged particles ranging from protons to lithium ions, which is illustrated in Fig. 1a. Good separation of all particles is obtained over their entire energy range. Since the energy resolution of each individual detector varies with the particle type, the particle identification cuts are defined to cover 3$`\sigma `$, where $`\sigma `$ is the standard deviation of the energy resolution of each particle type. Typical energy resolutions of the thin $`\mathrm{\Delta }E`$ detectors are between 40 and 80 keV, increasing with particle mass. The corresponding values are between 150 and 550 keV for the thick $`\mathrm{\Delta }E`$ detectors and between 900 and 1200 keV for the $`E`$ detectors. For energy depositions in the $`E`$ detector above 70 MeV in Fig. 1b, the two-dimensional cuts for protons, deuterons and tritons overlap slightly since the energy loss of the hydrogen isotopes in the $`\mathrm{\Delta }E_2`$ detector is rather small. This ambiguity is resolved by a two-dimensional plot (inset of Fig. 1b) of the deviations of the $`\mathrm{\Delta }E_1`$ and $`\mathrm{\Delta }E_2`$ signals from tabulated energy loss values in silicon  (solid lines in Fig. 1a). Particle identification is done by cutting along the minimum contour line, and thus possible misidentification should even out. This technique is also used to improve the separation between 3He and alpha particles in some telescopes where the energy resolution is poor.

Energy calibration of all detectors is obtained from the data itself . Events in the $`\mathrm{\Delta }EE`$ bands are fitted with respect to the energy deposited in the three detectors (solid lines in Fig. 1). This energy is determined from the detector thicknesses and tabulated energy loss values in silicon . The $`\mathrm{\Delta }E_1`$ detectors are further calibrated and checked using a 5.48 MeV alpha source. For the energy calibration of the CsI(Tl) detectors, two parameterizations of the light output versus energy of the detected particle  are used, one for hydrogen isotopes and another one for helium isotopes. Supplementary calibration points are provided by the H(n,p) reaction, as well as transitions to the ground state and low-lying states in the 12C(n,d)11B and 28Si (n,d)27Al reactions. The energy of each particle type is obtained by adding the energy deposited in each element of the telescope.

Low-energy charged particles are stopped in the $`\mathrm{\Delta }E_1`$ detector leading to a low-energy cutoff for particle identification of about 3 MeV for hydrogen isotopes and about 8 MeV for helium isotopes (see Fig. 1a). The helium isotopes stopped in the $`\mathrm{\Delta }E_1`$ detector are nevertheless analyzed and a remarkably low cutoff, about 4 MeV, can be achieved for the experimental alpha-particle spectra. These alpha-particle events could obviously not be separated from 3He events in the same energy region, but the yield of 3He is much smaller than the alpha-particle yield in the region just above 8 MeV, where the particle identification works properly. That the relative yield of 3He is small is also supported by the theoretical calculations in the evaporation peak region. In conclusion, the 3He yield is within the statistical uncertainties of the alpha-particle yield for alpha energies between 4 and 8 MeV. A consequence of this procedure is that the 3He spectra have a low-energy cutoff of about 8 MeV.

### 3.2 Low-energy neutron rejection and background subtraction

Knowing the energy calibration and the flight distances, the flight time for each charged particle from target to detector can be calculated and subtracted from the registered total TOF. The resulting neutron TOF is used for selection of charged-particle events induced by neutrons in the main peak of the incident neutron spectrum. The TOF cut reduces the background of charged particles produced by peak neutrons hitting the chamber and telescope housing since the flight paths are different, especially for the backward telescopes. The widths of the TOF cuts in all detectors are fixed to 3$`\sigma `$ where $`\sigma `$ is the standard deviation of the H(n,p) peak in the $`20^{}`$ telescope. Fig. 2a illustrates the selection procedure for deuterons at $`20^{}`$ laboratory angle. The solid line is a kinematic calculation of the ground state peak in the deuteron spectra for each corresponding neutron energy. It provides a cross check of the energy and time calibration of the whole energy spectrum.

Background events, measured in target-out runs and analyzed in the same way as target-in events, are subtracted from the corresponding target-in runs after normalization to the same neutron fluence. Fig. 2b shows the resulting spectrum of deuteron events at $`20^{}`$ induced by the main neutron peak. For comparison, the same spectrum without TOF cut is presented. Finally, the target-out background, obtained with the same TOF cut is shown. The signal-to-background ratio is about 4.

### 3.3 Absolute cross section normalization

Absolute double-differential cross sections are obtained by normalizing the silicon data to the number of recoil protons emerging from the CH2 target. After selection of events in the main neutron peak and proper subtraction of the target-out and 12C(n,p) background contributions, the latter taken from a previous experiment, the cross section can be determined from the recoil proton peak, using $`np`$ scattering data . All data have been normalized using the $`np`$ scattering peak in the $`20^{}`$ telescope. As a cross check, Si(n,px) spectra have also been normalized using the $`np`$ scattering peak in the $`40^{}`$ and $`60^{}`$ telescopes, resulting in spectra in agreement with those normalized to the $`20^{}`$ telescope.

## 4 Corrections

### 4.1 Thick target correction

Due to the thickness of the target and to the low-energy cutoffs in the particle identification, the measured low-energy charged particles are produced in fractions of the entire thickness of the target. Therefore, not only energy-loss corrections are needed but also particle-loss corrections. Charged particles with the initial kinetic energy $`E_{init}`$ have a well-defined range $`R`$ in the target material. If $`R(E_{init})`$ is equal to or larger than the target thickness, all produced particles can escape from the target and no particle loss correction is required. If, on the other hand, $`R(E_{init})`$ is smaller than the target thickness, a correction for particles stopped inside the target is needed.

The adopted correction method employs an initial energy $`(E_{init})`$ distribution called the inverse response function for each measured energy. For the 303 $`\mu `$m silicon target used in the present experiment, a measured alpha particle of 4 MeV could either be due to a 4 MeV particle from the front surface of the target, a 27 MeV particle from the back surface of the target, or anything in between. Therefore, the content of the measured energy bin should be redistributed over the initial energy region from 4 to 27 MeV. A FORTRAN program, TCORR , has been developed which calculates the inverse response functions, initially assuming an energy-independent cross section. These inverse response functions are normalized to the corresponding bin content in the measured spectrum and summed to get the true initial energy spectrum. Finally, the particle loss correction is applied. The resulting spectrum is folded with the primary inverse response functions to get improved inverse response functions and the procedure is repeated. Resulting spectra from two successive iterations are compared by a Kolmogorov test  to judge the convergence.

Results from the correction method have been verified with an independent Monte-Carlo program called TARGSIM, based on the GEANT code . This program simulates the measured spectra using the corrected spectra and the MEDLEY geometry as input. The simulation results are in agreement with the experimental data within the statistical errors over the whole energy region.

Obviously, the simulated spectra have much better statistics than the original experimental spectra and, therefore, the statistical fluctuations between neighboring energy bins are much smaller. In a sense, they are fits to the experimental spectra. In order to estimate the systematic uncertainty introduced by the thick target correction, these simulated spectra are corrected with TCORR again and compared with the result of the first correction. The observed differences for individual energy bins are typically 5 % and less than 10 % in general. An extreme value of 40 % was found in the lowest bin of the alpha spectrum at $`140^{}`$. However, in all cases, except for protons where the statistical errors are very small, the deviations are within the statistical uncertainties of the original corrected data.

In conclusion, the systematic error of the target correction comes essentially from the statistical uncertainties. For protons and deuterons we estimate that this error is about 10 % in the lowest two energy bins decreasing to a few percent from 15 MeV and upwards. Due to less statistics and the increasing width of the inverse response functions, the uncertainty is larger for tritons, 3He and alpha particles, where it is 20 % in the lowest two bins, decreasing to 10 % above 25 MeV.

In addition, evaluated data  were used as input to check the reliability of our programs, obviously because validation with known realistic data is desirable. The latter have been simulated with the TARGSIM program to get pseudo-experimental data and have subsequently been corrected with the TCORR program using the same conditions as in the experiment. The corrected results appear to reproduce the known realistic data well.

### 4.2 Collimator correction

As mentioned in sect. 2, active collimators have been placed in front of the telescope in order to define the solid angle. However, due to malfunctioning in the present experiment, the signal from these collimators could not be used to suppress events hitting them. Therefore, although the collimators actually work as passive collimators for helium particles below 35 MeV, their effect when particles punch through them has to be corrected for. To this end, a FORTRAN program has been developed that, based on the measured spectrum of particles and an iteration procedure, estimates the shape and fraction of the energy spectrum of particles hitting the collimator. It has been found that the corrections in shape are rather small and under control in all cases. The systematic error related to this correction comes from the uncertainty in the solid angle subtended by the silicon detectors for high-energy protons relative to the solid angle subtended by the collimator opening. This uncertainty is estimated to be 5 % and, due to the normalization procedure, only affects the helium spectra and the low-energy part of the hydrogen spectra.

### 4.3 Other corrections

The 17 MHz repetition rate of the cyclotron beam pulse, which limits the TOF window to 58 ns, causes wrap-around problems. Thus, it is not possible to distinguish 96 MeV neutrons from those of 26 MeV created by the previous beam burst, since the latter have the same apparent TOF. This can be seen in Fig. 2a, where the bent band from the low-energy neutron tail crosses the straight band of the full-energy neutrons. Since the Q-value for the 28Si(n,d) reaction is $`9.4`$ MeV, this interference shows up as a bump below 20 MeV in Fig. 2b. A correction for this effected is applied, using tabulated values from Ref.  and a ratio of the neutron fluence in the wrap-around region and at 96 MeV of 6.3 %. For the neutron-energy spectrum in the wrap-around region, a square distribution ranging from 24 to 29 MeV is assumed. Thus, the cross sections at 24, 26 and 28 MeV as given in Ref.  are used, with the 24 MeV values entering at half weight. The data for 80, 100, 120, 140 and 160 degrees are obtained by linear interpolation. Only the spectra for proton, deuteron and alpha particles are corrected. The effect of this correction is a reduction of about 5 % in the production cross section. In the (n,d) spectra presented in Fig. 4, some structure at $`20^{}`$ and $`40^{}`$ around 15 MeV might be attributed to deficiencies in the correction. The triton production cross sections given in Ref.  (Q-value = -16.2 MeV) indicate, that the correction would be about an order of magnitude lower and is therefore negligible. For 3He production (Q-value = -12.1 MeV), the correction is also negligible due to the high-energy cutoff of 8 MeV.

There is a TOF shift problem, seen as a band parallel with the main band in Fig. 2a. The reason for this is probably that the electronic timing module has not worked properly. This is corrected by extending the TOF cut with the dotted rectangle in the same figure, to include these events. This method could be applied only in the energy region where there is no interference from the low energy neutron tail. Therefore, the ratio of the number of events between the parallel and the main band is determined and then applied to the low-energy region as well. This ratio is 1.3 % in the worst case.

Albeit a majority of the neutrons appears in the narrow full-energy peak at 95.6 MeV, a significant fraction (about 25 %) belongs to a tail extending towards lower energies, remaining also after the TOF cut. The average neutron energy with these tail neutrons included is 92.4 MeV. This effect has been taken into account in the normalization of the data.

Minor corrections of a few percent are applied to the experimental spectra for the CsI(Tl) intrinsic efficiency  and for the dead time in the data acquisition system.

## 5 Theoretical models

Data have been compared with nuclear theory predictions, computed with the two nuclear reaction codes GNASH  and TALYS . While GNASH has been widely used during the last years, TALYS is a new code still under development. Two sets of GNASH calculations are presented, one with parameters as presented in a recent evaluation , and another set with modified parameters  as described in sect. 5.2. The latter parameter set is developed as part of another data evaluation . Since the latter work and TALYS are not published, they are described in some detail below.

Both GNASH and TALYS integrate direct, pre-equilibrium, and statistical nuclear reaction models into one calculation scheme and thereby give predictions for all the open reaction channels. Both codes use the Hauser-Feshbach model for sequential equilibrium decay and the exciton model for pre-equilibrium emission. The angular distributions are obtained using the Kalbach systematics .

### 5.1 TALYS calculations

The purpose of TALYS is to simulate nuclear reactions that involve neutrons, photons, protons, deuterons, tritons, 3He and alpha particles, in the 1 keV – 200 MeV energy range. Predicted quantities include integrated, single- and double-differential cross sections, for both the continuum and discrete states, residue production and fission cross sections, gamma-ray production cross sections, etc. For the present work, single- and double-differential cross sections are of interest. To predict these, a calculation scheme is invoked which consists of a direct + pre-equilibrium reaction calculation followed by subsequent compound nucleus decay of all possible residual nuclides calculated by means of the Hauser-Feshbach model.

First, dedicated optical model potentials (OMP) were developed for both neutrons and protons on 28Si up to 200 MeV. The used parameters are from the OMP collection of Ref. . These potentials provide the necessary reaction cross sections and transmission coefficients for the statistical model calculations. For complex particles, the optical potentials were directly derived from the nucleon potentials using the folding approach of Watanabe .

Pre-equilibrium emission takes place after the first stage of the reaction but long before statistical equilibrium of the compound nucleus is attained. It is imagined that the incident particle step-by-step creates more complex states in the compound system and gradually loses its memory of the initial energy and direction. The default pre-equilibrium model of TALYS is the two-component exciton model of Kalbach . In the exciton model (see Refs.  and  for extensive reviews), at any moment during the reaction, the nuclear state is characterized by the total energy $`E_{tot}`$ and the total number of particles above and holes below the Fermi surface. Particles ($`p`$) and holes ($`h`$) are indiscriminately referred to as excitons. Furthermore, it is assumed that all possible ways of sharing the excitation energy between different particle-hole configurations with the same exciton number $`n=p+h`$ have equal probability. To keep track of the evolution of the scattering process, one merely traces the development of the exciton number, which changes in time as a result of intranuclear two-body collisions.

The basic starting point of the exciton model is a time-dependent master equation, which describes the probability of transitions to more and less complex particle-hole states as well as transitions to the continuum, i.e., emission. Upon integration over time, the energy-averaged emission spectrum is obtained. The assumptions above make the exciton model amenable to practical calculations. This, however, requires the introduction of a free parameter, namely the average matrix element of the residual two-body interaction, occurring in the transition rates between two exciton states. Without going into details, the basic formulae are given for the two-component exciton model. The created particles and holes of proton and neutron type are explicitly followed throughout the reaction. A notation is used in which $`p_\pi (p_\nu )`$ is the proton (neutron) particle number and $`h_\pi (h_\nu )`$ the proton (neutron) hole number. Following Kalbach , the exciton model cross section is now given by

$$\frac{d\sigma _k^{EM}}{dE_k}=\sigma ^{CF}\underset{p_\pi =p_\pi ^0}{\overset{p_\pi ^{eq}}{}}\underset{p_\nu =p_\nu ^0}{\overset{p_\nu ^{eq}}{}}w_k(p_\pi ,h_\pi ,p_\nu ,h_\nu ,E_k)S_{pre}(p_\pi ,h_\pi ,p_\nu ,h_\nu ),$$
(1)
where $`\sigma ^{CF}`$ is the compound formation cross section and $`S_{pre}`$ the time-integrated strength which determines how long the system remains in a certain exciton configuration . The initial proton and neutron particle numbers are denoted $`p_\pi ^0=Z_p`$,and $`p_\nu ^0=N_p`$ with $`Z_p(N_p)`$ being the proton (neutron) number of the projectile. In general, $`h_\pi =p_\pi p_\pi ^0`$ and $`h_\nu =p_\nu p_\nu ^0`$, so that the initial hole numbers are zero, i.e. $`h_\pi ^0=h_\nu ^0=0`$, for primary pre-equilibrium emission. The pre-equilibrium part is calculated by Eq. 1, using $`p_\pi ^{eq}=p_\nu ^{eq}=6`$, whereas the remainder of the reaction flux is distributed through the Hauser-Feshbach model. In addition, the never-come-back approximation is adopted.

The emission rate $`w_k`$ for ejectile $`k`$ with spin $`s_k`$ is given by

$$w_k(p_\pi ,h_\pi ,p_\nu ,h_\nu ,E_k)=\frac{2s_k+1}{\pi ^2\mathrm{}^3}\mu _kE_k\sigma _{k,inv}(E_k)\frac{\omega (p_\pi Z_k,h_\pi ,p_\nu N_k,h_\nu ,E_x)}{\omega (p_\pi ,h_\pi ,p_\nu ,h_\nu ,E^{tot})},$$
(2)
where $`\sigma _{k,inv}(E_k)`$ is the inverse reaction cross section as calculated from the optical model and $`\omega `$ is the two-component particle-hole state density. The expression for $`S_{pre}`$ contains the adjustable transition matrix element $`M^2`$ for each possible transition between neutron-proton exciton configurations. A proton-neutron ratio of 1.6 for the squared internal transition matrix elements was adopted to give the best overall agreement with experiment, i.e., $`M_{\pi \nu }^2=M_{\nu \pi }^2=1.6M_{\pi \pi }^2=1.6M_{\nu \nu }^2`$. Partial level density parameters $`g_\pi =Z/15`$ and $`g_\nu =N/15`$ were used in the equidistant spacing model for the partial level densities.

At incident energies above several tens of MeV, the residual nuclides formed after binary emission may have so large excitation energy that the presence of additional fast particles inside the nucleus becomes possible. The latter can be imagined as strongly excited particle-hole pairs resulting from the first binary interaction with the projectile. The residual system is then clearly non-equilibrated and the excited particle that is high in the continuum may, in addition to the first emitted particle, also be emitted on a short time scale. This so-called multiple pre-equilibrium emission forms an alternative theoretical picture of the intra-nuclear cascade process, whereby the exact location and momentum of the particles are not followed, but instead the total energy of the system and the number of particle-hole excitations (exciton number).

In actual calculations, the particle-hole configuration of the residual nucleus after emission of the ejectile, is re-entered as initial condition in Eq. 1. When looping over all possible residual configurations, the multiple pre-equilibrium contribution is obtained. In TALYS, multiple pre-equilibrium emission is followed up to arbitrary order, though for 96 MeV only secondary pre-equilibrium emission is significant.

It is well-known that semi-classical models, such as the exciton model, have always had some problems to describe angular distributions (essentially because it is based on a compound-like concept instead of a direct one). Therefore, as mentioned previously, the double-differential cross sections are obtained from the calculated energy spectra using the Kalbach systematics .

To account for the evaporation peaks in the charged-particle spectra, multiple compound emission was treated with the Hauser-Feshbach model. In this scheme, all reaction chains are followed until all emission channels are closed. The Ignatyuk model  has been adopted for the total level density to account for the damping of shell effects at high excitation energies.

For pre-equilibrium reactions involving deuterons, tritons, 3He and alpha particles, a contribution from the exciton model is automatically calculated with the formalism described above. It is, however, well known that for nuclear reactions involving projectiles and ejectiles with different particle numbers, mechanisms like stripping, pick-up and knock-out play an important role and these direct-like reactions are not covered by the exciton model. Therefore, Kalbach developed a phenomenological contribution for these mechanisms , which is included in TALYS. It has recently been shown (see Table I of Ref. ) that this method gives a considerable improvement over the older methods. The latter seemed to consistently underpredict neutron-induced reaction cross sections.

### 5.2 GNASH calculations

For the present work, GNASH calculations have been performed with a modified parameter set. The calculation procedure is outlined in Ref. . Transmission coefficients needed for the GNASH input were calculated using the optical potential parameters by Sun et al.  for neutrons and protons, Daehnick et al.  for deuterons, Becchetti-Greenlees  for tritons and 3He particles, and Avrigeanu et al.  for alpha particles.

Like in the TALYS case, default level density parameters were used with the Ignatyuk level density formula . The normalization factor used in the pre-equilibrium model calculation was determined by analyses of proton-induced reactions. The calculated result of pre-equilibrium deuteron and alpha emission is different from that of the original GNASH code calculation . In the deuteron emission, the component with the exciton number 3 was ignored. The direct pick-up component was calculated using a phenomenological approach  with a normalization that is independent of the incident energy. This normalization was determined from analysis of experimental (n,dx) energy spectra up to 60 MeV . The alpha knockout component given by the same phenomenology  was ignored.

The results are given in the laboratory system. Like in the TALYS case, angular distributions are obtained using the Kalbach systematics . The required pre-equilibrium fraction is taken from the GNASH output. The c.m.-to-lab transformation is performed using the kinematics of one-particle emission as described in Refs. .

The exciton model implemented in GNASH is a one-component exciton model developed by Kalbach , with a parameterisation for the energy dependence of the squared internal transition matrix element which has been validated at relatively low incident energies (below 40 MeV). There are indications that at higher incident energies, this energy dependence is no longer appropriate and that a more general form, covering a wider energy range, is needed. Such a smooth form has been implemented in TALYS, on the basis of a collection of double-differential (nucleon-in,nucleon-out) cross section measurements .

## 6 Results and discussion

Double-differential cross sections at laboratory angles of $`20^{}`$, $`40^{}`$, $`100^{}`$ and $`140^{}`$ for protons, deuterons, tritons, 3He and alpha particles are shown in Figs. 37, respectively. All spectra for each particle type are plotted on the same cross section scale to facilitate the comparison of their magnitude. The choice of the energy bin width is a compromise between the energy resolution in the experiment, the width of the inverse response functions and acceptable statistics in each energy bin. The error bars represent statistical uncertainties only.

The overall relative statistical uncertainties of individual points in the double-differential energy spectra at $`20^{}`$ are typically 3 % for protons, 7 % for deuterons, 20 % for tritons, 20 % for 3He and 15 % for alpha particles. As the angular distributions are forward-peaked, these values increase with angle. The systematic uncertainty contributions are due to thick target correction ($`120`$ %), collimated solid angle ($`15`$ %), beam monitoring ($`23`$ %), the number of silicon nuclei (1 %), CsI(Tl) intrinsic efficiency (1 %), particle identification (1 %) and dead time ($`<`$ 0.1 %). The uncertainty in the absolute cross section is about 5 %, which is due to uncertainties in the $`np`$ scattering angle, the contribution from the low-energy continuum of the 7Li(p,n) spectrum to the $`np`$ scattering proton peak (3 %), the reference $`np`$ cross sections (2 %) , statistics in the $`np`$ scattering proton peak (2 %), the carbon contribution (0.1 %) and the number of hydrogen nuclei (0.1 %).

From Figs. 37 it is obvious that the charged-particle emission from 96 MeV neutron irradiation of silicon is dominated by proton, deuteron and alpha particle channels. The spectra of the two other particle types studied in this work (tritons and 3He) are more than an order of magnitude weaker. All the spectra have more or less pronounced peaks at low energies (below $`1015`$ MeV), the angular distributions of which are not too far from isotropy. This low-energy peak is not observed in the 3He spectra due to the 8 MeV low-energy cutoff discussed in sect. 3.1.

All the particle spectra at forward angles show relatively large yields at medium-to-high energies. The emission of high-energy particles is strongly forward-peaked and hardly visible in the backward hemisphere. It is a sign of particle emission before statistical equilibrium has been reached in the reaction process. In addition to this broad distribution of emitted particles, the deuteron spectra at forward angles show narrow peaks corresponding to transitions to the ground state and low-lying states in the final nucleus, 27Al. These transitions are most likely due to pick-up of weakly bound protons in the target nucleus, 28Si.

### 6.1 Comparison with theoretical model calculations

In Figs. 38 the experimental results are presented together with theoretical model calculations. The GNASH calculations of Ref.  have been done for protons, deuterons and alpha particles, whereas the other two calculations have been performed for all five particle types.

Fig. 3 shows a comparison between the double-differential (n,px) experimental spectra and the calculations based on the TALYS and GNASH models. For protons above 25 MeV, all calculations give a good description of the spectra. Below this energy, some differences can be observed, e.g., at forward angles TALYS gives a better description of the statistical peak than the GNASH calculations.

The situation is quite different for the deuteron spectra (Fig. 4). None of the predictions do account for the data. At all angles deviations of a factor of two or more are present. At forward angles the high-energy part is strongly overestimated, indicating problems in the hole-strength treatment. There is a large difference in the spectral shapes calculated with the two versions of GNASH . This difference is due to the fact that emission from the configurations with exciton number 3 is neglected in the present GNASH calculations. This component is taken into account as a direct pickup component calculated with an empirical formula due to Kalbach .

For tritons (Fig. 5), the TALYS calculations give a slightly better description of the experimental data, whereas for 3He (Fig. 6) some large deviations can be observed. The TALYS calculations seem to account better for the spectrum shapes.

The overall description of the alpha particle spectra (Fig. 7) is fair. The GNASH calculations overpredict the high-energy data at forward angles, whereas the TALYS predictions are too large at backward angles.

The ability of the models to account for the low-energy peak caused by evaporation processes is not impressive. In general, the models tend to overpredict the cross sections. It should, however, be kept in mind that the peak maximum is close to (for 3He below) the low-energy cutoff, which complicates the comparison. Another complication in this context is that the c.m.-to-lab transformation of the calculated TALYS spectra could, at least in some cases, make a considerable difference. The GNASH cross sections are given in the lab system, but the c.m.-to-lab transformation is performed using the kinematics of one-particle emission , which obviously is an approximation.

### 6.2 Integrated spectra

For each energy bin of the light-ion spectra, the experimental angular distribution is fitted by a simple two-parameter functional form, $`a\mathrm{exp}(b\mathrm{cos}\theta )`$ .

This allows extrapolation of double-differential cross sections to very forward and very backward angles. In this way coverage of the full angular range is obtained. By integration of the angular distribution, energy-differential cross sections ($`d\sigma /dE`$) are obtained for each ejectile. These are shown in Fig. 8 together with the theoretical calculations. All calculations are in good agreement with the proton experimental data over the whole energy range. In the cases of deuterons and alpha particles, the models overpredict the high-energy parts of the spectra.

The production cross sections are deduced by integration of the energy-differential spectra (see Table 1). As explained above, the experimental values in Table 1 have to be corrected for the undetected particles below the low-energy cutoff. This is particularly important for 3He because of the high cutoff.

The proton and deuteron production cross sections are compared with previous data at lower energies  in Figs. 9 and 10. There seems to be general agreement between the trend of the previous data and the present data point. The curves in these figures are based on a GNASH calculation .

## 7 Conclusions and outlook

In the present paper, we report an experimental data set on light-ion production induced by 96 MeV neutrons on silicon. Experimental double-differential cross sections ($`d^2\sigma /d\mathrm{\Omega }dE`$) are measured at eight angles between $`20^{}`$ and $`160^{}`$. Energy-differential ($`d\sigma /dE`$) and production cross sections are obtained for the five types of outgoing particles. Theoretical calculations based on nuclear reaction codes including direct, pre-equilibrium and statistical calculations give generally a good account of the magnitude of the experimental cross sections. For proton emission, the shape of the spectra for the double-differential and energy-differential cross sections are well described. The calculated and the experimental alpha-particle spectra are also in fair agreement with the exception of the high energy part, where the theory predicts higher yields than experimentally observed. For the other complex ejectiles (deuteron, triton and 3He) there are important differences between theory and experiment in what concerns the shape of the spectra.

For the further development of the field, data at even higher energies are requested. The results suggest that the MEDLEY facility, which was used for the present work, should be upgraded to work also at 180 MeV, i.e., the maximum energy of the TSL neutron beam facility. At present, a new neutron beam facility is under commissioning at TSL, covering the same energy range, but with a projected intensity increase of a factor five. This will facilitate measurements at higher energies than in the present work.

The setup described in this paper comprises an active target, the information of which was not used in the analysis here but can provide valuable information on the kinetic energy transferred to the residual nucleus. This information might be crucial for soft-error studies and therefore it is of interest to compare this measurement with theoretical calculations. Work along this line is in progress.

## Acknowledgments

This work was supported by the Swedish Natural Science Research Council, the Swedish Nuclear Fuel and Waste Management Company, the Swedish Nuclear Power Inspectorate, Ringhals AB, and the Swedish Defence Research Agency. The authors wish to thank the The Svedberg Laboratory for excellent support. One of the authors (U.T.) wishes to express his gratitude to the Thai Ministry of University Affairs and to the International Program in the Physical Sciences at Uppsala University. One of the authors (Y.W.) is grateful to the scientific exchange program between the Japan Society for the Promotion of Science and the Royal Swedish Academy of Sciences.

## Figure captions

1. (a) Particle identification spectra at $`20^{}`$ for the $`\mathrm{\Delta }E_1\mathrm{\Delta }E_2`$ (a) and $`\mathrm{\Delta }E_2E`$ (b) detector combinations. The solid lines represent tabulated energy loss values in silicon . The insert in (b) illustrates the separation of high-energy protons, deuterons and tritons discussed in sect. 3.1.
2. (a) Neutron TOF spectrum versus deuteron energy for the Si(n,dx) reaction at $`20^{}`$ and the selection of deuterons associated with the full-energy neutron peak. The neutron-energy scale is given to the right. The solid line is a kinematic calculation of the ground-state deuteron energy as a function of the neutron energy. The lower rectangular cut is associated with neutrons in the full-energy peak, whereas the adjacent rectangular cut is used when correcting for the observed timing shift discussed in sect. 4.3. (b) Deuteron energy spectrum at $`20^{}`$ with (solid histogram) and without (dashed histogram) the full-energy neutron cut. The cross-hatched histogram shows the target-out background. The bump below 20 MeV in the solid histogram is due to wrap-around effects discussed in sect. 4.3.
3. Experimental double-differential cross sections (filled circles) of the Si(n,px) reaction at 96 MeV at four laboratory angles. The curves indicate theoretical calculations based on GNASH  (dashed), TALYS-present work (dotted) and GNASH-present work (solid). The TALYS result is in the c.m. system and the GNASH results are in the lab system.
4. Experimental double-differential cross sections (filled circles) of the Si(n,dx) reaction at 96 MeV at four laboratory angles. The curves indicate theoretical calculations based on GNASH  (dashed), TALYS-present work (dotted) and GNASH-present work (solid). The TALYS result is in the c.m. system and the GNASH results are in the lab system.
5. Experimental double-differential cross sections (filled circles) of the Si(n,tx) reaction at 96 MeV at four laboratory angles. The curves indicate theoretical calculations based on TALYS-present work (dotted) and GNASH-present work (solid). The TALYS result is in the c.m. system and the GNASH result is in the lab system.
6. Experimental double-differential cross sections (filled circles) of the Si(n,3Hex) reaction at 96 MeV at four laboratory angles. The curves indicate theoretical calculations based on TALYS-present work (dotted) and GNASH-present work (solid). The TALYS result is in the c.m. system and the GNASH result is in the lab system.
7. Experimental double-differential cross sections (filled circles) of the Si(n,$`\alpha `$x) reaction at 96 MeV at four laboratory angles. The curves indicate theoretical calculations based on GNASH  (dashed), TALYS-present work (dotted) and GNASH-present work (solid). The TALYS result is in the c.m. system and the GNASH results are in the lab system. Note the logarithmic scale.
8. Experimental energy-differential cross sections (filled circles) for neutron-induced p, d, t, 3He and $`\alpha `$ production at 96 MeV. The curves indicate theoretical calculations based on GNASH  (dashed), TALYS-present work (dotted) and GNASH-present work (solid). The TALYS result is in the c.m. system and the GNASH results are in the lab system.
9. Neutron-induced proton production cross section as a function of neutron energy. The full circle is from the present work, whereas the open circles are from previous work . The curve is based on a GNASH calculation . The data as well as the calculations correspond to a cutoff energy of 4 MeV. Note that the cutoff energy is different from that in Table 1.
10. Same as Fig. 9 for deuteron production, with a cutoff energy of 8 MeV.