FLNR Annual Report 2022

      The construction of new and the upgrade and optimization of the existing accelerators of the DRIBs-III complex continued in 2022.

DC-280

      The basic facility of the SHE Factory, the DC-280 cyclotron, provided 6000 h of beamtime for research in 2022, including 4000 h for experiments on the synthesis of superheavy elements and study of their chemical properties using the DGFRS-2 and GRAND set-ups.
After adjusting the acceleration modes for 48Ca, 54Cr, and 48Ti ions, the intensity of the accelerated beams was 7.73 pµA for 48Ca, 3.8 pµA for 54Cr, and 2.13 pµA for 48Ti. To reduce time for maintenance and to make the cyclotron operation more reliable, the components that duplicated those requiring regular service were manufactured. The currently used deflector was improved, and a new tool with an upgraded structure was manufactured and commissioned. Moreover, a reserve buncher block was fabricated. The commissioning of the flat-top system and beam phase motion monitor system is currently underway.

U-400M

      As part of the U-400M upgrade, work on the cyclotron magnetic system was completed magnetic field strength measured by generating a magnetic field map first harmonic of the magnetic field corrected using a special set of shims; valley shims added for increasing the magnetic field at the extraction radius. Furthermore, a new magnetic channel for the extraction system was developed and manufactured, a vacuum chamber was assembled and tested, RF generators were upgraded, and a new vacuum pumping system was assembled. The windings for the correction coil were fabricated in collaboration with the specialists from the Department for Superconducting Magnet Research and Technologies of the 9eksler and Baldin Laboratory of High Energy Physics.

U-400

      A wide variety of scientific and applied investigations in heavy-ion physics were conducted using the U-400 cyclotron. In 2022, the cyclotron provided over 6400 h of beamtime. Experiments with the beams of 6Li (MA9R), 16O (CORSET), 22Ne (9ASSILISSA),

48Ca (CORSET, 9ASSILISSA, MA9R, SHELS), 24, 26Mg (CORSET, SHELS), 90Zn and 209Bi (CORSET) were carried out. Some experiments were dedicated to applied research with the beams of Ne, Ar, Kr, and Bi ions.

IC-100

      The IC-100 cyclotron, used for applied research, provided over 2500 h of beamtime. Ions from O to Xe accelerated at IC-100 up to the energies of 1.0– 1.2 MeV/nucleon were used for irradiating the samples of graphene, AlN, Si3N4, MgO, MgAl2O4, ODS steeles, high-temperature titan-based superconductors (in collaboration with the South Africa, Poland, Serbia, Belarus, Kazakhstan, and the Czech Republic), and for in situ studies of the optical properties of radiation-resistant dielectrics under ion irradiation.

MT-25

      The MT-25 electron accelerator ran for 1200 h. The facility was employed in irradiation of biological samples for the Laboratory of Radiation Biology of JINR and 9orone]h State University. Electron components were tested in cooperation with NIIKP and SPE Detector LLC. The promising potential for the use of rare-earth oxides as matrices in practical applications, such as the disposal of radioactive waste, was explored in collaboration with N.I.Lobachevsky State University of Nizhny Novgorod. In addition, ceolits were studied in cooperation with a group of researchers from 9ietnam. In a Joint effort with the Dzhelepov Laboratory of Nuclear Problems of JINR, methods for measuring the electron energy were worked on.

DC-140

      The implementation of the DC-140 project for applied research at FLNR is ongoing [1]. The premises of Building 101 were prepared for constructing a new accelerator complex and allocating engineering systems. The design documentation was prepared for building the premises, allocating and integrating engineering systems of the new accelerator complex into the existing infrastructure. Construction documents for the cyclotron components and experimental set-ups are ready. The equipment is manufactured, some being already constructed and delivered to FLNR.

Experiment at the Dubna Gas-Filled Recoil Separator (DGFRS-2)

      A series of experiments was carried out using the gas-filled separator DGFRS-2 of the Factory of Superheavy Elements at FLNR JINR. The studies of the reaction of 48Ca with 243Am target nuclei were continued with a view to thoroughly exploring the properties of Mc isotopes and their daughter nuclei and measuring the reaction excitation function in a wide 48Ca beam energy range (Fig.1). A new 286Mc isotope was synthesized, and the cross section for the 5n evaporation channel was measured. Four new decay chains of 289Mc (2n channel), 55 decay chains of 288Mc (3n channel), and four decay chains assigned to 287Mc (4n channel) were detected. In addition, the spontaneous fission of 279Rg was observed for the first time. The α decay of 268Db was confirmed, its branch and half-life being more precisely specified. The decay properties of 21 isotopes from 287–289Mc to 266–268Db, including those of 264Lr, were measured with greater precision.

    First experiments on the synthesis of Ds isotopes in the 232Th+48Ca reaction were conducted. Their properties are crucial for identifying new element 120 in the reactions 249Cf(50Ti,3–4n) 295,296120 and 245Cm(54Cr, 3–4n) 295,296120 because the α decays of nuclei under consideration lead to the 275,276Ds isotopes. Moreover, the predicted fission barriers of the 232Th+48Ca reaction products, governing the survival probability of excited compound nuclei, are lower than those of the isotopes of element 120. The cross section for the reaction with 232Th target nuclei will

allow more accurate predictions of the production cross sections for the isotopes of element 120. Six decay chains of the new isotope 276Ds were synthesi]ed for the first time at two 48Ca beam energies. The α decay of 276Ds led to the discovery of two more isotopes, 272Hs and 268Sg (Fig.1). The reaction cross sections were 70 fb and 0.7 pb at the projectile energies of 231 and 238 MeV, respectively. The results of the experiments are presented in [2–5].

Spectroscopy of Heavy and Superheavy Nuclei

      Following the replacement of the first triplet of quadrupole lenses of the SHELS separator, first test experiments were conducted aimed at defining the separation efficiency of reaction products formed in complete fusion reactions of the 22Ne, 40Ar, 48Ca ions with the target nuclei of Pb and U. Figure 2 shows a comparison of spectra in the focal plane of the separator prior to and after the replacement. As is seen, the background conditions were substantially improved. It should be noted that an increase in the transmission did not exceed 5%.

    The novel GABRIELA-2 detection system comprising five “clover” high-purity germanium γ detectors was assembled and will help determine with record efficiency the characteristics of γ transitions in heavy short-lived nuclei synthesized at SHELS. Having a minimum tranformation time of 1 μs, the electronic CAMAC-based data acquisition system was replaced with a digital detection system from National Instruments.

The novel system whose distinctive feature is a minimum transformation time of 8 ns provides an advantage in detecting the exotic short-lived states of excited nuclei. New components of the detection system were tested using the 26Mg+206Pb complete fusion reaction, which is of peculiar interest owning to the formation of a new isotope 227Pu in the 5n evaporation channel. Experimental results are processed.

Chemistry of Transactinides

      In 2022, preparations were well advanced for the first experiments aimed at studying the chemical properties of superheavies. The GRAND separator (DGFRS-) was commissioned, key separator systems were tested, and transmission was measured (50% for such reactions as 48Ca+206,208Pb). In addition, the cryodetector was tuned using the 40Ar and 48Ca beams.

      First experiments were carried out at the novel experimental complex of the SHE Factory combining the physics separator (GRAND) and a chemical setup (a cryodetector). We pursued studies of the Fl behaviour, presumably in the elemental state, by gas adsorption thermochromatography during irradiation at the DC-280 heavy-ion accelerator. The shortlived radionuclide 287Fl with a half-life T1/2=0.36 s was synthesized online in the 242Pu(48Ca, 3n) 287Fl reaction. Reaction products were preseparated using the new gas-filled GRAND separator and collected in a gas catcher, a recoil transfer chamber installed in the focal plane and separated from the gas volume of the separator by a thin mylar film. Only highly volatile elements (e.g., Hg, Rn) or their compounds were transported from the gas catcher at a temperature of 20°C to the chemical set-up via a teflon capillary in a carrier gas, a mixture of additionally purified inert gases He/Ar. As a preseparator for the cryodetector, GRAND allowed by 3–4 orders of magnitude better purity of separated Fl atoms from unwanted byproducts (short-lived isotopes of transplutonium elements). This significantly improves the statistical reliability of spectometric data, setting a new standard for SHE chemistry research. In addition, the preseparator allowed one to place the cryodetector measurement system near the focal plane of the

separator and the detecting module at a minimum possible distance of 25 cm from the gas catcher, thereby reducing the time needed for gas transport to the chemical detector to 0.1 s. Volatile Fl atoms were studied by adsorption thermochromatography on the surface of gold-plated semiconductor detectors in the He/Ar gas mixture over the temperature range from 20°C to –170°C. For this purpose, a linear temperature gradient of –6°C/cm was obtained for the first time in the thermochromatographic module of the cryodetector. In research at DC-280 in December, two decay chains of 287Fl were detected in the cryodetector at the temperatures of approximately –100°C and –70°C, which preliminary confirms the previously made conclusions about the high volatility and chemical inertness of elemental Fl. The analysis of the experimental data is pursued. A mobile adsorption model developed at FLNR and the acquired chromatographic data will allow conclusions to be made regarding the thermodynamic properties of Fl.

Dynamics of Heavy-Ion Interaction, Fission of Heavy and Superheavy Nuclei

      In 2022, mass and energy distributions of fragments formed in the 54Cr+208Pb, 232Th, 238U reactions were measured at near-barrier energies for determining the probability of complete fusion of nuclei under investigation. The analysis of the experimental data showed that in transitioning from 48Ca to 54Cr incident ions, the formation probability of a compound nucleus decreases by more than two orders of magnitude in all the reactions under consideration.
      A systematic investigation of the properties of fusion–fission and quasifission was made on the basis of a comprehensive analysis of the experimental data reported earlier in [6]. By analyzing experimental mass distributions, asymmetric quasifission was found to occur over time scales of 5–7 zs in systems with Z₁Z₂<2000, whereas in those with Z₁Z₂>2000, the lifetime of the composite nuclear system was found to decrease with increasing Z₁Z₂ (Fig.3)
      Multimodal fission studies continued. The proton structures at Z=36 and Z=45 were found to affect the formation of fission fragments of neutron-deficient pre-actinide nuclei (178Pt, 180,182,183Hg,

      184Pb) [7]. In studying the fission properties of heavy acntinide nuclei 248Cf, 254,256Fm at an excitation energy of 40–60 MeV, a multimodal fission was found to manifest at all measured excitation energies, though the liquid-drop behaviour dominated. The structural peculiarities of mass and energy distributions attributed to shell effects become less prominent exponentially as the excitation energy of the fissioning nucleus increases [8].
Pursued are the studies of multinucleon transfer reactions that could provide a means of synthesizing new, first and foremost neutron-rich isotopes of transuranium elements [9]. The results of the theoretical modeling revealed the regularities in the dependence of the cross sections for the synthesis of new nuclei on the reaction partners, energy, and detection angles, which have to be taken into consideration when planning experiments.

Structure of Exotic Nuclei

      First experiments at the novel ACCULINNA-2 fragment separator [10] were of decisive importance in nuclear physics in that they resulted in the detection of superheavy 6H and 7H isotopes [11, 12] resolving one of the key issues that has long been posing challenges to experimentalists and thereby allowing advancements in the exploration of a new mode of spontaneous nuclear decay accompanied by a simultaneous emission of four neutrons.
Suggested earlier in [11], a technique for setting up the experiment allowed the studies of the states in 6H populated via the 2H(8He, 4He)6H reaction [12]. Analogous to 7H, the detection of 4He in coincidence with high-energy tritons was assumed to serve an indicator of one or several sequential 6H decays. The reference measurement of the 2H(10Be, 4He)8Li reaction confirmed the effectiveness of the method used for studying the mechanism of the (d,α) reaction. The missing mass spectrum of 6H was recon-

structed from low-energy 4He recoils detected in coincidence with 3H and neutrons. The simulations and data showed that the energy resolution in the missing mass spectrum was better than 2 MeV. Thereto, record-breaking statistics for the 6H system was collected in the experiment [12]: over 4000 double 4He–3H coincidences and about 130 triple 4He–3H–n coincidences. In the reconstructed 6H spectrum, an important finding was the absence of possible states at the energy E_T<3.5 MeV above the 3H+3n decay threshold. This result disagrees with those from previous experiments [Aleksandrov D. V. et al. Observation of Nonstable Heavy Hydrogen Isotope 6H in the Reaction 7Li(7Li, 8B) // Yad. Fi. 1984. V.39. P.513] that reported for the first time on the observation of the 6H resonance state at the energy E_T=2.7(4) MeV. A bump observed in previous studies may be accounted for by an order of magnitude higher cross section for populating the 5H ground state in the 7Li(7Li, 9B*)5H reaction.
After processing the experimental data by using the correlation analysis, with due regard for triple 4He–3H–n coincidences, two possible states of the 6H isotope were found at E_T~4.5 (g.s.) and 6.8 MeV. The previously proclaimed 6H ground state at ~2.6–2.9 MeV above the 3H+3n threshold was not observed in the experiment involving the 2H(8He,4He)6H reaction with a cross section limit dσ/dΩ_cm5μb/sr. A scheme of levels and decays of the 7H and 6H isotopes (Fig.4) obtained in the experiments [11, 12] allows a conclusion that the decay of the 7H ground state may be accompanied by a simultaneous emission of four neutrons (a “true” five-particle decay 3H+4n).

This is the first proven case for the existence of such a nuclear decay mode.

Reactions with Beams of Light Stable and Radioactive Nuclei

      In 2022, two experiments were conducted at the U-400 cyclotron employing the high-resolution magnet analyser MAVR. In an experiment with the beams of the 48Ca and 56Fe ions accelerated to 10 MeV/nucleon and directed to the Au and 238U tar-

gets, the differential cross sections were measured for the emission of alphas and other light charged particles at an angle of 0°. The spectra revealed fast α particles with energies close to the kinematic limit for the two- and three-body exit channels. Correlation experiments with fission fragments pointed out the possibility of forming weakly excited heavy nuclei in the reactions under

consideration. The analysis of the experimental data using a moving source model indicated several sources for the formation of high-energy nonequilibrium particles. The mechanism of the emission of nonequilibrium α particles from the target nucleus could be attributed to complete or incomplete fusion of nuclei. The main experimental results were published in [13, 14].

Construction of a Separator Based on Resonance Laser Ionization (GaLS Set-Up)

      The GALS set-up under construction is intended for the separation and study of the products of multinucleon transfer reactions. The following main results were achieved in 2022: 1. A novel reaction chamber was manufactured to search for and study the optimal levels of atomic transitions for optimal ioni]ation efficiency. In addition, a transport system based on grid electrodes and a registration system were constructed. The upgrade of the evaporative laser for the reference chamber of the GALS set-up is on track to be completed. 2. A detailed scheme on the basis of CAEN software and electronic components were developed for the detection system of the GALS set-up.

All the necessary electronic components and primary configuration control programmes were purchased. The mechanical part of the tape station was manufactured in collaboration with iThemba LABS (South Africa). 3. A lab for off-line experiments was prepared, including the installation of engineering systems (power supply, a distillate system, a gas system, etc). A scheme was developed for guiding optical beams within the laser laboratory and for transmitting laser radiation to new experimental set-ups. A possibility of transporting laser radiation from the laser lab to the experimental set-ups by using optical fibers was analy]ed. The required single- and multimode fiber sets were chosen and technical specifications were outlined for the sets and inputoutput devices.

Gas Ion Catcher

      The construction of the cryogenic gas ion catcher, a new set-up for the SHE Factory, continued in 2022. The warm and cold vacuum chambers of the catcher were assembled and evacuated to a pressure of less than 10^–7 Torr. The multi-electrode system for transporting reaction products to the supersonic nozzle was assembled. The copper sheath of the cold chamber, including the gas cooling coil, was manufactured and installed. The system of vacuum pumping control and temperature control of the cold chamber (and the gas in it) was assembled and debugged. Designed for measuring the composition of residual gases in the gas cell, a system based on the mass spectrometer PrismaPro (Pfeiffer) was adMusted. The cooling system of the inner chamber was launched, and a temperature of 48 . was attained at a helium pressure of 10 mbar.
By using specially developed software and performing simulations, the efficiency and extraction time from the cryogenic gas ion catcher were determined for products synthesized in the

following complete fusion reactions: 40Ar+144Sm→ 184Hg*, 40Ar+166Er → 206Rn*, 48Ca+197Au→ 245Es*, 48Ca+208Pb→ 256No*, 48Ca+209Bi→ 257Lr*, 48Ca+242Pu→ 290Fl*. To test the gas catcher without a beam by using an α source, the efficiency and the extraction time of the α decay daughter products were measured.
In collaboration with the Institute for Analytical Instrumentation of RAS (Saint Petersburg) and under a grant from the Ministry of Science and Higher Education of the Russian Federation No. 075-10-2020-117 (“Superheavy Nuclei and Atoms: Mass Limits of Nuclei and the Borders of Mendeleev’s Periodic Table” [15]), work continues on the design of the multiple-reflection time-of-flight mass spectrometer intended for the precision measurement of the isotope masses of heavy and superheavy nuclei. In 2022, a preliminary design was completed. Tender documents for manufacturing the mass spectrometer are being prepared. A contract for fabricating a calibrant ion source of the mass spectrometer is underway.

      Using high-resolution transmission electron microscopy and computer simulation (molecular dynamics), the parameters of latent tracks in nano- (n-Si₃N₄) and polycrystalline (p-Si₃N₄) silicon nitride were determined in a wide range of electronic stopping levels [16]. The effects of the formation of swift heavy-ion tracks in the Si₃N₄ and AlN crystals and in nanocrystalline Y₄Al₂O₉ and Y₂Ti₂O₇were also studied.
      The mechanical properties of ODS steels irradiated with swift heavy ions were determined by small specimen compression testing whose results showed that strength properties depended on the structural state of material.
      A target device was fabricated for uniform ion doping of metal samples with helium using a method based on the in-depth stop zone scanning of accelerated ions. The device was designed for producing samples for subsequent TEM studies of the structural changes in reactor materials simulated by helium implantation under long-term neutron irradiation.
      Heavy-ion irradiation was established to result in the formation of nanopores and ultra-long nanochannels in graphene oxide of nearly any thickness: from single-layer graphene oxide to films of several microns in thickness. The pores of films comprising over 3–4 layers are cylindrical, on average having a narrow size distribution of ~ 6 nm. The experimental studies and modeling by reactive molecular dynamics showed that the pore size depends, to a significant extent, on the composition and the functionalization degree of graphene oxide and on the electron ion energy loss. The pore periphery is electrically conductive owning to the partial restoring of the graphitic structure and contains nitrile groups [17].
      Pursued were the studies of the properties of track ion-selective membranes [18, 19] aimed at deep understanding of the mechanism governing the formation of ion-selective channels in polyethylene terephthalate films irradiated with heavy ions and subjected to mild photolysis. The results are crucial for the development of membranes for efficient ion separation.
      Track-etched membranes with ultra-small pores were used in experiments aimed at fulfilling

tasks related to the structure of electrical double layer in nanopores. Time-resolved measurements of streaming potential were performed. The surface charge density and a number of properties of a hypothetical gel layer on the pore walls of track-etched membranes were defined in the framework of the space charge model. A successful attempt was made for the first time to employ highly asymmetric tracketched membranes in the liquid–liquid membrane contractor. The studies paved the way for further developments of novel membrane purification and separation technologies.
      A technology was developed for producing a composite material comprising a track membrane and a layer of polymer nanofibers made from chitosan, collagen, and polylactide. An intermediate layer of titanium provides the adhesion of the fiber layer to the track membrane. The functionalization of the nanofiber layer with various agents gives composite membranes specific properties, thereby allowing their use in energy-saving water purification technologies, in regenerative medicine applications, such as next-generation wound dressings, and in cellular engineering practical applications [20].
      For studying membrane distillation, composite track membranes coated with a 500-nm-thick super hydrophobic polytetrafluoroethylene layer by electron beam dispersion were developed. The track membranes proved to be highly selective in desalinating sodium chloride aqueous solution.
      Research continued in the production of modified track membranes that can be used as flow sensors based on the surface-enhanced Raman scattering (SERS). Indeed, the track membranes coated with thin layers of silver by magnetron and thermal sputtering followed by self-assembly of nanoparticles due to the heat treatment have high gain coefficients of an order of 10–6 with respect to the compounds under investigation. Furthermore, immobilization of aptamers on membrane surfaces, affine to the proteins of the influenza A virus, allows the detection of up to 4×10³ viral particles per a millimeter using SERS, which is comparable to the sensitivity of a PCR test.

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