Fragmentation of the 4He2 dimer by relativistic highly charged projectiles in collisions with small kinetic energy release
Abstract
We study theoretically the fragmentation of the helium dimer, 4He2, into singly charged ions in collisions with relativistic highly-charged projectiles. We discuss the main mechanisms driving this process with the focus on the fragmentation caused by direct ionization of both atomic sites of the dimer in a single collision with the projectile. This direct mechanism dominates the He2 He+ + He+ breakup events with the kinetic energies of the emerging ionic fragments below – eV. We explore the energy and angular distributions of the He+ ions produced in collisions with and GeV/u U92+ projectiles and show that their shape is significantly affected by relativistic and higher-order effects in the interaction between the projectile and the dimer. We also show that the shape of the energy spectrum is quite sensitive to the binding energy of the He2 dimer which can be exploited for its precise determination. The contribution of the direct mechanism to the total cross section for the He2 fragmentation by and GeV/u U92+ was calculated to be Mb and Mb, respectively, representing roughly half of this cross section.
I Introduction
The study of fast ion-atom and ion-molecule collisions has already a long history. However, collisions of fast ions with very extended atomic objects, like humongous van der Waals dimers, are very rarely considered, even though compared to the ’normal’ case the physics of such collisions possesses new and interesting features.
In particular, to our knowledge there are just few papers, He2_alpha-particle -He2-rel-HCI-lett , where collisions of fast ions with the He2 and Li-He dimers were studied. In He2_alpha-particle -thesis_He2_S14+ and He2-rel-HCI-lett the fragmentation process He2 He was explored for collisions with different projectiles and at different impact velocities while in He-Li-rel-HCI single ionization of the Li-He dimer by ultra-fast projectiles involving energy transfer between the dimer atoms was considered.
Both the He2 and Li-He dimers are spectacular pure quantum systems. For instance, in the He2 dimer the interaction between two ground-state helium atoms is so weak that it supports one bound state only, which has an extremely small binding energy ( eV, e-l ). The size of this two-atomic bound system is enormous: its average bond length is Å e-l and the dimer extends to the distances of more than Å, being the largest known ground-state diatomic molecule. The outer classical turning point in the ground state of the dimer is about Å 14A that is almost four times smaller than its average bond length showing that the He2 dimer is a quantum halo system which spends most of the time in the classically forbidden region. Because of its enormous size the inter-atomic interaction and the dimer binding energy are noticeably influenced by the Casimir-Polder retardation effect Cas-Pol , retard .
When the He2 interacts with external electromagnetic fields a multitude of various processes becomes possible. They include a fragmentation of the He2 dimer into helium ions which may occur when the dimer is irradiated by an electromagnetic wave or bombarded by charged projectiles. Helium ions repeal each other that results in a Coulomb explosion of the system. The kinetic energy of the ionic fragments, which is released in this explosion, depends on their charges and the initial distance between them. The spectra of the kinetic energy release may contain a valuable information about the structure of the initial He2 dimer as well as transient dimers (which may be formed if the time interval between the interaction with the external field and the start of the Coulomb explosion is sufficiently large). Some of these fragmentation processes have been already studied.
The fragmentation of the He2 dimer into He+ ions, caused by absorption of a single photon, was considered in He2_photon - He2_photon_icd-calc . In dimer-binding-exp the process of He2 fragmentation into He+ ions, induced by absorption of two high-frequency photons, was employed to sample the dimer wave function at inter-atomic distances Å that enabled the authors to accurately measure the binding energy of the dimer.
The process of He2 fragmentation into singly charged ions in collisions with keV/u alpha particles and MeV/u S14+ projectiles was explored in He2_alpha-particle and He2_S14+ -thesis_He2_S14+ , respectively, where the focus was on the fragmentation events with kinetic energies of the He+ ions greatly exceeding eV.
Very recently, the process of He2 fragmentation in collisions with relativistic highly charged projectiles was considered in He2-rel-HCI-lett . Unlike He2_alpha-particle and He2_S14+ -thesis_He2_S14+ , in He2-rel-HCI-lett the fragmentation events with kinetic energies of He+ ions not significantly exceeding eV were explored. In particular, it was shown in He2-rel-HCI-lett that the lower-energy part of the fragmentation spectrum can be very strongly influenced by relativistic effects caused by the collision velocity approaching the speed of light and that the calculated energy spectrum is quite sensitive to the value of the dimer binding energy which can be exploited for measuring this energy.
In the present paper we continue to study the fragmentation reaction He2 He+ e- in relativistic collisions with highly charged ions. Like in He2-rel-HCI-lett , we will focus here on the fragmentation mechanism in which the projectile directly ionizes both helium atoms in a single collision. At relativistic collision velocities this mechanism becomes very long-ranged and, therefore, is especially suited to probe the ground state of the He2 at inter-atomic distances a.u., where it already completely dominates the fragmentation process.
The paper is organized as follows. The next section begins with a discussion of the main fragmentation mechanisms which are present in collisions with relativistic highly charged ions. Then we consider a theoretical description of the direct fragmentation mechanism mentioned above. In section III we present our results for the fragmentation cross sections. Section IV contains main conclusions.
Atomic units () are used throughout unless otherwise is stated.
II General consideration
II.1 The main fragmentation mechanisms
Let the He2 dimer collide with a projectile, which has a charge and moves with a velocity whose magnitude approaches the speed of light a.u. At the parameter , characterizing the effective strength of the projectile field in the collision, is well below , which indicates that the field of the projectile in the collision is on overall weak rather than strong. Consequently, the breakup of the He2 will occur with a non-negligible probability only provided the number of ’steps’ in the interaction of the projectile with the constituents of the dimer is reduced to a necessary minimum. Also, in relativistic collisions with very light atoms the processes of radiative and nonradiative electron capture from the atom by the projectile are already extremely weak having cross sections which are by several orders of magnitude smaller that atomic ionization and excitation cross sections el-cpt ; eic ; we-1998 ; He-ioniz .
The above features inherent to high-energy collisions with light targets restrict the number of the main fragmentation mechanisms, which govern the breakup of the He2 dimer into He+ ions
(1) |
by high-energy charged projectiles, to four He2-rel-HCI-lett .
II.1.1 Mechanisms of the ’delayed’ fragmentation
Two of these mechanisms can be termed as ’delayed’ since the average time, which they require for the formation of the He+–He+ system, is determined by the motion of the helium nuclei and, therefore, exceeds by several orders of magnitude the time, which is needed by the projectile to traverse the region of space occupied by the initial He2 dimer. These mechanisms are also characterized by relatively large values of the kinetic energy of the He+ fragments. Both of them involve the interaction between the projectile and just one site of the He2 dimer.
a) In the first of these mechanisms the collision between the projectile and one of the helium atoms results in its double ionization. Then the He2+–He system evolves until the He2+ radiatively captures one electron from the neutral helium atom and the resulting He+– He+ system undergoes a Coulomb explosion. This mechanism – according to its steps – can be denoted as double-ionization–radiative-electron-transfer (DI-RET).
The fragmentation cross section for this mechanism can be evaluated as , where is the cross section for double ionization of the helium atom by the projectile and the probability for radiative electron transfer. In relativistic collisions with very highly charged projectiles () the cross section reaches several tens of megabarns which in turn results in the magnitude of the of the order of megabarn (see subsection D of section III).
Within the reflection approximation, the kinetic energy of the ionic fragments, which is released in a Coulomb explosion, is related to the inter-nuclear distance at which the explosion started: in particular, for singly charged ions one has . The experimental results of dimer-binding-exp and the theoretical consideration of we-21-reflect-appr show that in the case of He2 the reflection approximation is quite accurate up to very low energies ( meV) where it starts to be violated by the recoil effects.
Since radiative electron transfer occurs only at small inter-nuclear distances (not exceeding a few atomic units) the DI-RET mechanism leads to fragmentation with relatively large kinetic energy release: the results of He2_alpha-particle and thesis_He2_S14+ show that in collisions with fast charged projectiles the energy spectrum of the fragments, which are produced via this mechanism, is peaked at eV corresponding to a.u., and that its intensity rapidly decreases when the energy departures from this value.
b) In the second ’delayed’ fragmentation mechanism the projectile also interacts with just one helium atom. Now, however, the interaction results in simultaneous ionization-excitation of this atom. In the presence of a neutral helium atom the excited helium ion can de-excite not only via spontaneous radiative decay but also by transferring energy to the neutral He atom that leads to ionization of the latter.
Such an energy transfer acquires a relatively large effective range becoming quite efficient if the He+ ion is produced in an excited state which can decay to the ground state by an electric dipole transition. Then the energy transfer occurs mainly via dipole-dipole two-center electron transitions.
To our knowledge, a radiationless relaxation of an excited atom via energy transfer to a neighbor atom, which at large inter-atomic distances occurs predominantly via the dipole-dipole interaction, was first considered theoretically in i-a-a . In the process, which was studied in i-a-a and termed there inter-atomic Auger decay (IAAD), the exited atom has initially a vacancy which is filled by its electron, but – unlike in ’normal’ (intra-atomic) Auger decay – the energy release is transferred to the neighbor atom ionizing it. The process of IAAD was shown in i-a-a to be so efficient that it can even outperform intra-atomic Auger decay.
In i-a-a also a simple approximate formula was derived for the IAAD rate . Being adapted to the case under consideration, the formula reads
(2) |
Here, is the rate for spontaneous radiative decay of the excited state of the He+ ion, is the energy difference between the excited and ground states of the He+ ion which is transferred to the He atom, is the cross section for single ionization of the He atom by absorption of a photon with frequency , is the distance between the He+ and He, and is a numerical parameter depending on the magnetic quantum number of the excited state of the He+.
The process of IAAD in a system of two atomic particles, where relaxation via intra-atomic Auger decay is not allowed energetically, was computed in icd and was called there interatomic coulombic decay (ICD). Nowadays the term ICD is often used to denote relaxation mechanisms, where an overlap between electronic shells of the interacting particles is not required since the energy is transferred via the exchange of virtual photons between them. Accordingly, the fragmentation mechanism, in which simultaneous ionization-excitation of one of the atoms by the projectiles is followed by ICD decay, can be denoted as IE-ICD.
The process of ICD in the He+–He system competes with spontaneous radiative decay, which does not result in the production of the second helium ion. Using Eq. (2) and assuming for definiteness that the excited He+ ion was produced in a –state we obtain for the ratio , where . This indicates that when the distance between the He+ and He significantly exceeds a.u. the ICD channel becomes inefficient (in the experiment He2_photon_icd on the He2 photo fragmentation the ICD was clearly ’visible’ up to a.u.). According to the results of He2_alpha-particle and thesis_He2_S14+ in fast collisions with charged projectiles the IE-ICD is very efficient in producing He+ ions with energies in the vicinity of eV, but is in essence completely inactivated above eV and below – eV. As rough estimates suggest (see subsection D of section III), in relativistic collisions with very highly charged projectile the sum of the contributions and to the total fragmentation cross section may rich few megabarns.
c) The average size of the He2 dimer greatly exceeds not only the effective range of RET but also that of ICD. Therefore, there must occur a very significant contraction of the intermediate (He+)∗–He and He2+–He dimers before the distance between the nuclei sufficiently decreases in order for the ICD and RET to come into the play. The contraction is possible because the potential of the He2+–He and (He+)∗–He systems at large inter-nuclear distances is attractive.
II.1.2 Mechanisms of the ’instantaneous’ fragmentation
In collisions with high-energy projectiles there are two more fragmentation mechanisms in which, unlike the DI-RET and IE-ICD, the He+-He+ system emerges ’instantaneously’, i.e. on the so short time scale that during the production of two helium ions the helium nuclei remain essentially at rest.
a). In one of them the projectile interacts with both atoms of the dimer. As a result, each helium atom emits an electron and becomes a singly charged ion. In this fragmentation mechanism the projectile directly forms the He+ - He+ system Sulf which undergoes a Coulomb explosion. Since the size of the He2 is very large, the interactions between the constituents of the dimer play in this mechanism no noticeable role. In He2-rel-HCI-lett this mechanism was termed the direct fragmentation (DF) and we shall use it also here.
We note that at relativistic impact velocities the time interval between the collisions of the projectile with the first and second atoms of the He2 dimer does not exceed few atomic units ( s). This is by orders of magnitude smaller than typical nuclear times (– s) in the He+ – He system, showing that the DF mechanism is indeed ’instantaneous’.
b). In the other ’instantaneous’ fragmentation mechanism the projectile interacts with just one atom of the dimer. As a result of this interaction, the atom emits an electron. There is a certain probability that the emitted electron will move towards the other atom and knock out one of its electrons. Thus, this fragmentation mechanism is a combination of single ionization of the helium atom by a high-energy projectile and the so called e-2e process on helium (single ionization by electron impact). Following He2-rel-HCI-lett we shall refer to this mechanism as single ionization – e-2e (SI–e-2e) f1 .
In the SI–e-2e process the velocity of the first emitted electron is by two orders of magnitude smaller than the velocity of the relativistic projectile. Nevertheless, this electron still moves much faster than the helium nuclei. With its typical velocity a.u., we obtain that the time, which the electron needs to propagate between the sites of the dimer, does not exceed s. Since this time is much shorter than typical nuclear times in the He+ – He system, the SI–e-2e mechanism can be also viewed as ’instantaneous’.
Since in both the DF and SI–e-2e the helium ions emerge at ’frozen’ positions of the helium nuclei, their energy is very simply () related to the size of the He2 dimer at the collision instant (as long as the recoil effects can be ignored, see subsection B of the present section).
The cross section for the production of two singly charged helium ions by relativistic projectiles via the DF mechanism depends on the transverse size of the He2 dimer He2-rel-HCI-lett , scaling approximately as . The corresponding cross section for the production via the SI–e-2e depends on the dimer size as He2-rel-HCI-lett .
Thus, unlike the DI-RET and IE-ICD, the DF and SI–e-2e mechanisms are not only instantaneous, providing a simple correspondence between the kinetic energy release and the size of the He2 dimer, but also possess much longer effective range. Therefore, they are especially suited for probing the ground state of the He2 in a very large interval of the inter-atomic distances .
Our calculations show that in collisions of He2 dimers with very highly charged projectiles () the DF mechanism is much more efficient than the SI–e-2e yielding cross sections which are larger by two orders of magnitude. Therefore, in the rest of the paper we shall concentrate on the He2 fragmentation via the DF mechanism.
II.2 The direct fragmentation mechanism
We shall consider collisions between the He2 dimer and the projectile using the semi-classical approximation in which the relative motion of the heavy particles (nuclei) is treated classically whereas the electrons are considered quantum mechanically.
We choose a reference frame in which the dimer is at rest and take the nucleus of one of its atoms as the origin. We shall refer to this atom as atom whereas the other will be denoted by . In this frame, the coordinates of the nucleus of atom are given by the inter-nuclear vector of the dimer and the projectile moves along a classical straight-line trajectory , where is the impact parameter with respect to the nucleus of atom and the collision velocity.
Since the size of the He2 dimer is very large, the ionization of atoms and occurs independently of each other and we can use the independent electron approximation. According to it the probability for single ionization of atoms and in the collision where the projectile moves with an impact parameter is given by
(3) |
Here, and are the probabilities for single ionization of atoms and , respectively, and is the collision impact parameter with respect to atom , where is the part of the inter-nuclear vector of the dimer which is perpendicular to the projectile velocity .
Within the independent electron approximation the probabilities for single ionization of helium atoms and read
(4) |
where () is the probability to remove one electron from helium atom in the collision with a projectile having an impact parameter () new-approach .
The quantity
(5) | |||||
represents the cross section for the production of two singly charged helium atom by the projectile in the collision with the He2 dimer at a given inter-nuclear vector of the latter. Since the probabilities and depend just on the absolute value of the respective impact parameters, and , the cross section (5) depends only on the absolute value of the two-dimensional vector : .
In our calculations of the probabilities and we regarded the helium atom in its initial and final states as an effectively single-electron system, where the ’active’ electron moves in the effective field, created by the ’frozen’ atomic core consisting of the atomic nucleus and the ’passive’ electron. This field is approximated by the potential
where is the distance between the active electron and the atomic nucleus, and and param . We note that with this choice of and , almost coincides with the exact Hartree-Fock potential.
The cross section (5) can be only computed numerically and the computation is quite time consuming. However, a simple estimate can be obtained for this cross section at a.u. He2-rel-HCI-lett
(6) |
Here, and are the modified Bessel function A-S , is the adiabatic collision radius, where is the collision Lorentz factor, a.u. is the mean transition frequency for single ionization of a helium atom, and is a free (fit) parameter which is a very slowly varying function of param-C .
Taking into account that and if whereas at , it follows from Eq. (6) that at the cross section decreases with relatively slowly, , whereas at the decrease is already exponential. This means that the projectile is able to efficiently irradiate both atoms of the dimer only provided that the dimer transverse size does not exceed the adiabatic collision radius . Since , an ultrafast projectile possesses a very large effective interaction range and can probe systems with large dimensions. Simple estimates show that, beginning with impact energies of a few GeV/u, the adiabatic collision radius exceeds the size of the He2 dimer He2-rel-HCI-lett .
The cross section (5) refers to the situation where two helium atoms in the dimer are separated by the vector with the absolute value of its transverse projection . It yields an important information about the collisions giving an insight into the basic physics of the fragmentation process He2-rel-HCI-lett but cannot be (directly) measured in experiment. Therefore, let us ’convert’ the cross section (5) into quantities which can be measured. We start with the expression
(7) |
where is the wave function describing the relative motion of the atoms in the ground state of the He2 dimer.
As was already mentioned, we assume that before the collision with the projectile the He2 dimer was at rest. Let and be the recoil momenta of the helium ions, which they acquire during the collision because of the interaction with the projectile and electron emission, and let and be the final momenta of these ions after the Coulomb explosion. Then the energy conservation for the relative motion of the ionic fragments reads
(8) |
Here, is the final kinetic energy of the relative motion of the ionic fragments, and are the momentum of their relative motion and the reduced mass, respectively, and () are their charges and is the distance between the ions when the Coulomb explosion began and which in the case under consideration coincides with the size of the initial He2 dimer at the collision instant. In the energy balance (8) we have neglected the kinetic energy of the He+ ions, which they had due to the nuclear motion before the collision and which is very small because the depth of the potential well in the He2 dimer is just meV.
Since in the process of single ionization of helium atoms by relativistic projectiles the recoil momenta of the helium ions do not noticeably exceed a.u. rhci -r-sea , the first term on the right hand side of Eq. (8) is in the meV range. Such values are comparable to the Coulomb potential energy at the inter-nuclear distances of the order of a.u. which is much larger than the size of the He2 (and any known) dimer. Therefore, the neglect of the recoil energy, given by the first term on the right-hand side of Eq. (8), does not have any substantial impact on the energy balance. Thus, the relation
(9) |
between the kinetic energy release and the size of the dimer at the collision instant, which neglects the recoil energies, is expected to be very accurate down to energies meV.
Let us now make a more restrictive assumption that not only the recoil energies are much smaller than the Coulomb energy but also that the absolute values of the recoil momenta, and , of the fragments are significantly less than . Since these values do not exceed a.u. the assumption will be fulfilled beginning with – a.u. that corresponds to the energies meV. Under such conditions the momentum will be directed essentially along the inter-nuclear vector of the initial He2 dimer and, taking also into account (9), we get
(10) |
Using (7) and (9)-(10) we obtain the fragmentation cross section differential in the relative momentum of the ionic fragments
(11) | |||||
where , and is the polar angle of the momentum (the -axis is along the projectile velocity ). Since the bound state of the He2 dimer is spherically symmetric, the wave function does not depend on : .
Taking into account that , where is the azimuthal angle of , and that the right-hand side of Eq. (11) does not depend on we obtain the fragmentation cross section differential in the kinetic energy release and the polar angle
(12) | |||||
In our consideration of the direct fragmentation process, its two steps – ’instantaneous’ production of two He+ ions and the consequent Coulomb explosion of the He+–He+ system – are fully disentangled, even though the energy of the emitted electrons and the kinetic energy release have the same source: the energy transferred by the projectile to the He2 dimer. However, since the electrons emitted from helium atoms in collisions with relativistic projectiles have energies extending up to a few tens of eV whereas, as will be seen below, the spectrum of the kinetic energy release in the DF process peaks at eV and essentially vanishes already at – eV, such a consideration is expected to be quite accurate.
III Results and Discussion
III.1 Preliminary remarks
In this section we report our results for the fragmentation cross sections. In our calculations the ground state of the He2 dimer was described by a wave function corresponding to the dimer binding energy of neV (this value is very close to that given in 139.2 ): this wave function was used to get results presented below in figures 1-7. In addition, in order to explore the sensitivity of the cross sections to the value of , also wave functions corresponding to neV and neV were applied for obtaining results shown in figure 8.
Four different approximations were employed for computing the probabilities for single electron removal from a helium atom (see Eq. (4)). They include: i) the nonrelativistic first Born approximation (nr-FBA); ii) the nonrelativistic symmetric eikonal approximation (nr-SEA) nr-sea ; iii) the relativistic first Born approximation (r-FBA) and iv) the relativistic symmetric eikonal approximation (r-SEA) r-sea .
The differences between results obtained by using the first Born and symmetric eikonal approximations offer an idea about the importance of the higher-order effects in the interaction between the projectile and the atoms of the dimer. On the other hand, the differences between results of the relativistic and nonrelativistic approximations yield the information about the role of relativistic effects in the He2 fragmentation.
In particular, in the nr-FBA and nr-SEA the speed of light is assumed to be infinite which means that all relativistic effects caused by very high collision velocities vanish. In the r-FBA and r-SEA a.u. and relativistic effects arising due to high impact energies are taken into account. Since even in very high-energy collisions with helium targets the overwhelming majority of emitted electrons have energies well below eV we-jpb-2005 , the main relativistic effects, which are due to high impact energies and which may influence the He2 fragmentation, are caused by the deviation of the electric field of the projectile from the (unretarded) Coulomb form.
One should say that, in addition to relativistic effects due to high impact velocities, there are also relativistic effects in the ground state of the free He2 which – according to 139.2 – reduce the binding energy of the dimer by about . This affects the form of its wave function (especially at very large inter-atomic distances) that in turn may have an impact on the shape of the spectrum of the fragments He2-rel-HCI-lett .
III.2 Fragmentation spectra


In figures 1 and 2 we show the doubly differential cross section for the fragmentation of the He2 dimer into He+ ions occurring in collisions with GeV/u and GeV/u U92+ projectiles, respectively. The corresponding collision velocities and the Lorentz factor are a.u., and a.u., , respectively. The cross section is plotted as a function of the kinetic energy release and the fragmentation angle presenting a general picture of the fragmentation spectrum. Taking into account that the spectrum is symmetric with respect to the transformation , only the interval of angles is considered.
It is seen in these figures that the spectrum is predominantly localized in the energy interval eV eV and at fragmentation angles not significantly exceeding . It is also seen that at very small energies the spectrum is restricted to smaller fragmentation angles whereas with increasing the energy the spectrum shifts to larger .
The interval of kinetic energies eV eV corresponds to the instantaneous size of the He2 dimer during the collision in the range a.u. a.u. The probability to find the He2 dimer in this range is above that is reflected in the dominance of the above energy interval in the spectrum. At energies – eV the spectrum practically vanishes since they correspond to the inter-nuclear distances a.u., where the probability to find the He2 dimer is negligibly small.
The cross section for the production of two helium ions by the projectile decreases with the transverse size of the dimer at the collision instant ( at ). Since at a fixed the value of is proportional to , the fragmentation with very small may occur at very small only, whereas at significantly larger values of it becomes possible at not very small as well. Taking also into account that the cross section is proportional to the geometrical factor we can explain the ’shift’ of the spectrum to larger with increase in , which is observed in figures 1 and 2.
It also follows from the results presented in figures 1 and 2 that for collisions with so very highly charged projectiles, as U92 ions, the symmetric eikonal approximation predicts a noticeably smaller number of the fragmentation events. This shows that the higher-order effects in the interaction between the projectile and the target remain visible even at very high impact energies. The smaller cross section values, predicted by the symmetric eikonal approximation, reflects the general tendency that in high-energy collisions the higher-order effects reduce cross section values.


Figures 3 and 4 give a more detailed information about the fragmentation process by displaying the cross section as a function of the fragmentation angle at a given value of the kinetic energy release : meV, meV, eV and eV. Some conclusions can be drawn from the results presented in these figures.
First, by comparing results of the different calculations we see that the shape of the He2 fragmentation pattern is in general influenced by both relativistic effects, which arise due to collision velocities approaching the speed of light, and higher-order effects, which originate in a very high charge of the projectile.
Second, the influence of the relativistic effects increases when the kinetic energy release decreases: these effects especially impact the fragmentation events with very small kinetic energy release where they enhance the cross section up to one or two orders of magnitude. On the other hand, the fragmentation with larger values of is only very modestly influenced by these effects.
Third, the situation with the higher-order effects is just opposite: their role rises with increasing and they mostly affect the fragments having larger energies. However, even for such fragments these effects remains modest, reducing the cross section values not significantly more than -. The higher-order effects also somewhat influence the low-energy part of the spectrum: in this case, however, their effect is limited to the very small angles only.
The above qualitative features of the fragmentation process can be understood by noting that the cross section is most profoundly influenced by the relativistic effects when the magnitude of is large () whereas the higher-order effects are most significant in collisions where the projectile passes close to both atoms of the dimer (the impact parameters and do not exceed a few atomic units) that is possible only at relatively small values of .
Very large values of imply that the instantaneous dimer size in the collision has to be very large and, in addition, the dimer orientation angle should not be small. Since and , it follows that the relativistic effects are most significant for fragmentation events, which are characterized by a very small kinetic energy release and not too small angles .
On the other hand, collisions occurring at small values of , where the higher-order effects can be substantial, are characterized by either small values of the instantaneous dimer size or very small angles (or a combination of both). The kinetic energy release of eV, eV, eV and eV corresponds to a.u., a.u., a.u. and a.u., respectively. In order to have substantial higher-order effects at the first two values of the dimer has to be almost parallel to the collision velocity. As a result, in collisions with very small such effects can become visible only at the fragmentation angles close to zero whose contribution, due to the geometric factor , is very small. For collisions with larger the restrictions on the angle are not so strict and the higher-order effects may be noticeable for the whole range .
The energy of eV, eV, eV and eV correspond to the relative momentum of a.u., a.u., a.u. and a.u., respectively. The first two momentum values are not very large. Therefore, in the case of eV and eV the very narrow peak at very small angles (see panels () and () of figures 3–4) can be noticeably smeared out by the recoil effects.

In figure 5 we display the angular distribution of the He+ fragments represented by the cross section . The cross section was obtained by integrating either over the energy interval eV eV, in which the direct fragmentation mechanism is by far the dominant one, or over the broader range eV eV, which covers essentially all energies which are possible in the fragmentation events caused by this mechanism (see figures 1-2).
Figure 5 shows that the angular distribution of the He+ fragments becomes significantly weaker dependent on the angle when their energy increases. This feature (which is already seen in figures 3–4) can be understood by taking into account that, due to the relation , the He+ fragments with larger energies emerge when the projectiles hit the He2 dimers with smaller size . In such collisions the DF mechanism is more efficient causing the He2 breakup with significant probabilities even when the dimer is oriented at large angles with respect to the impact velocity.

The energy spectrum, , of He+ fragments produced by bombarding the He2 dimer by and GeV/u U92+ projectiles is displayed in figure 6. The spectrum shown in the left panels of this figure was obtained by integrating over all possible fragmentation angles, , whereas that given in the right panels includes only the fragments moving at large angles, , with respect to the projectile velocity.
The results shown in figure 6 confirm the correspondences between the relativistic and higher-order effects and the energy and angle of the fragments which were discussed above. In particular, we again observe that at a given collision velocity the relativistic effects rise when the energy decreases, becoming especially strong in collisions where the He+ fragments possess quite small energies and move at large angles with respect to the projectile velocity.

In figure 7 we compare the energy spectra of the He+ ions produced in collisions with and GeV/u U92+ and MeV/u S14+ ( a.u., ). It is seen that the shape of the spectrum profoundly varies with an increase in the impact energy. In particular, the maximum of the energy distribution is shifted from eV in collisions with MeV/u S14+ to eV in collisions with GeV/u U92+ where the low-energy part of the spectrum is strongly enhanced (see figure 7a) and this enhancement becomes even much more pronounced if the fragmentation events with large angles are selected (figure 7b).
In collisions with MeV/u S14+ and GeV/u U92+ the effective strength of the projectile field, given by the ratio , is essentially the same ( and , respectively). Therefore, the strong enhancement of the lower-energy part of the fragmentation spectrum, which reflects the corresponding strong increase in the breakup of dimers with very large instantaneous size , is caused by a much higher impact energy. One should note, however, that since He2 is a very light target, a large increase in the collision velocity has a more profound overall effect on the spectrum shape and the total number of events than an increase in the Lorentz factor .
III.3 The energy spectrum shape versus the He2 binding energy

The values for the binding energy of the He2 dimer, reported in the literature, vary between neV 44.8 and neV 161.7 . The distribution of the probability density in the ground state of the dimer depends on the value of and a variation in the binding energy would be reflected by the corresponding variation of the probability density . However, if is relatively small, , a large range of has to be spanned in order for the changes in the shape of to become noticeable.
In this respect, as it was already emphasized in He2-rel-HCI-lett , the fragmentation by ultra-fast projectiles can be of especial interest. Indeed, since the adiabatic collision radius increases with the impact energy as , they possess a very large effective interaction range that is a great advantage in probing the structure of such enormous objects like the He2 dimer.
In figure 8 we display the energy spectrum for the He2 fragmentation by GeV/u U92+. In the range of , shown in the figure, the direct fragmentation is by far the dominant breakup channel and the cross section represents the total energy spectrum.
The spectrum was calculated for three values of the dimer binding energy : neV, neV and neV. For a better visibility of the variation of the spectrum shape with , the spectra for neV and neV were normalized to the spectrum for neV at an energy meV.
In the energy interval, meV eV, the ratios , and vary by about , and , respectively. The corresponding relative variations, , of the binding energy are approximately , and , respectively. This means that in the energy interval under consideration the shape of the energy spectrum ’magnifies’ the variation of the binding energy by about three times.
A more detailed analysis of the cross sections shows that the range of quite small ( eV) gives the main contribution to the variation of the cross section ratios. This is not very surprising since the small energy range, meV eV, corresponds to a very large interval, a.u. a.u., of the interatomic distances in the He2 dimer, where the shape of its ground state becomes sensitive to even a very modest variation of the binding energy. The projectile is able to span in the collision so large interval of distances since at GeV/u the adiabatic collision radius a.u. already significantly exceeds the size of the dimer.
III.4 The total fragmentation cross sections
According to our r-SEA calculations, the contribution of the DF mechanism to the total cross section for the breakup of the He2 dimer in collisions with and GeV/u U92+ projectiles amounts to Mb and Mb, respectively.
The relativistic effects in the direct fragmentation are most significant when the ’instantaneous’ transverse size of the He2 dimer in the collision is very large. Consequently, they most profoundly influence the fragmentation events with small and large . However, such events have relatively small probabilities and, as a result, the cross section is very weakly influenced by the relativistic effects. In particular, for collisions with and GeV/u U92+ the difference between our results for , obtained using relativistic and nonrelativistic approaches, is about merely .
The field of the projectile acting on the dimer is strongest when the impact parameters with respect to both atomic sites of the dimer are small, i.e. in collisions where the ’instantaneous’ transverse size of the dimer is not large. Since such collisions give a more significant contribution to , than those with very large , the influence of the higher-order effects in the interaction between the projectile and the dimer on the magnitude of is substantially larger reaching about for the fragmentation by and GeV/u U92+.
In the present paper the He2 fragmentation via the IE-ICD and DI-RET mechanisms was not calculated. Nevertheless, we can still obtain a rough estimate for the contribution to the total fragmentation cross section due to these two mechanisms. According to the experimental results of thesis_He2_S14+ , in the breakup of the He2 dimer by MeV S14+ the ratio of the summed contributions of the IE-ICD and DI-RET channels to the contribution of the DF channel is approximately equal to . Taking into account that our calculation for the DF contribution in collisions with MeV/u S14+ yields Mb, we obtain that the summed contributions of the IE-ICD and DI-RET to the fragmentation by MeV S14+ is Mb.
The cross sections for the fragmentation via the IE-ICD and DI-RET are proportional to the cross sections for simultaneous ionization-excitation and double ionization, respectively, of the helium atom. Both these cross section scale similarly with and . Therefore, by calculating them for collisions with MeV/u S14+ and and GeV/u U92+ projectiles and using our results for the DF cross sections, we have estimated that the summed contribution of the IE-ICD and DI-RET mechanisms to the fragmentation in collisions with and GeV/u U92+ is roughly equal to Mb and Mb, respectively.
IV Conclusions
In conclusion, we have studied the fragmentation of the helium dimer into singly charged helium ions by relativistic highly charged projectiles in collisions with relatively low kinetic energy release – eV. Such breakup events occur solely due to the direct fragmentation mechanism in which the projectile ionized both dimer’s atoms in a single collision. In this mechanism the two helium ions are produced within the so short time interval ( s) that during the production the helium nuclei remain essentially at rest. Consequently, the energy of the ionic fragments, produced via the direct mechanism, is very simply () related to the size of the He2 dimer at the collision instant.
We have investigated in detail the energy and angular spectra of the He+ ions produced in collisions with and GeV/u U92+ projectiles. Our main findings can be summarized as follows.
In collisions with the fragmentation events, in which the He+ ions move with low kinetic energies ( eV) under large angles () with respect to the projectile velocity, are strongly affected by the relativistic effects.
The shape of the energy spectrum of the He+ ions is quite sensitive to the binding energy of the He2 dimer which can be exploited for its precise determination. Here the relativistic effects also play the important role since, by significantly enhancing the lower-energy part of the spectrum, they enable one to span a substantially broader range of the inter-atomic distances in the dimer, effectively increasing the sensitivity of the spectrum shape to the variation of the dimer binding energy.
The relativistic effects, having a strong impact on the fragments with low and large and making the energy spectrum shape more sensitive to the variation in the dimer binding energy, influence nevertheless very weakly the total amount of the fragmentation events caused by the direct mechanism because they affect only their minor part. In this respect, a large increase in the collision velocity has a much stronger overall effect on the spectrum shape and the total number of events.
In contrast to relativistic effects, the role of the higher-order effects in the projectile-dimer interaction rises with increasing energy of the He+ fragments becoming substantial at eV. Since such events give a more significant contribution to the fragmentation than those with very small , the influence of the higher-order effects is substantially larger reaching about for the total cross section in the direct fragmentation by and GeV/u U92+.
According to our calculations the contribution of the direct mechanism to the total cross section for the He2 fragmentation by and GeV/u U92+ amounts to Mb and Mb, respectively. A rough estimate for the total fragmentation cross section in these collisions, which takes into account all the fragmentation mechanisms, suggests that it is about two times larger than the above values.
Acknowledgements.
BN, SFZ and XM gratefully acknowledge the support from the ‘National Key Research and Development Program of China’ (Grant No. 2017YFA0402300) and the CAS President’s Fellowship Initiative. Our numerical results were obtained using the facilities of the Supercomputer Center HIRFL at the Institute of Modern Physics (Chinese Academy of Sciences).References
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