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1.
J Comput Chem ; 44(19): 1673-1689, 2023 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-37177883

RESUMO

Stabilizing the exotic chemical species possessing multiple bonds is often extremely challenging due to insufficient orbital overlap, especially involving one heavier element. Bulky aryl groups and/or carbene as ligand have previously stabilized the SiSi, GeGe, and BB triple bonds. Herein, theoretical calculations have been carried out to shed light on the stability and bonding of elusive silaboryne/germaboryne (Si/GeB triple bond) stabilized by donor base ligands ((cAAC)BE(Me)(L); E = Si, L = cAACMe , NHCMe , PMe3 ; E = Ge, L = cAACMe ). The heavier analogues (Sn, Pb) have been further studied for comparison. Additionally, the effects of bulky substituents at the Si and N atoms on the structural parameters and stability of those species have been investigated. Energy decomposition analysis coupled with natural orbital for chemical valence (EDA-NOCV; for Si) showed that cAAC/NHC ligands could stabilize the exotic BSi-Me species more efficiently than PMe3 ligands. The BSi partial triple bond of the corresponding species possesses a mixture of one covalent electron sharing BSi σ-bond and two dative π-bonds (B ← Si, B → Si).


Assuntos
Elétrons , Ligantes
2.
Int J Biol Macromol ; 221: 1053-1064, 2022 Nov 30.
Artigo em Inglês | MEDLINE | ID: mdl-36108744

RESUMO

Keeping in view the future prospectus of carbohydrate polymers, present research report is an elaboration, exploration and execution of the research expectancy in area of these polymers by researchers like John F. Kennedy. Herein, molecular interactions and physiochemical properties of modified bioactive arabinoxylan-psyllium have been evaluated for drug delivery applications. Arabinoxylan-psyllium was modified with sulphated and amide copolymers and co-polymers were characterized by SEMs, AFM, FTIR, XRD, solid state 13C NMR, TGA-DSC and water absorption studies. The 13C-NMR and FTIR confirmed grafted copolymers. The polymer-blood interactions revealed non-thrombogenic nature with thrombose percentage 63.17 ± 5.61 % and polymer-mucous membrane interactions showed detachment force 0.237 ± 0.078Nwith bio-membrane in mucoadhesion test. The pH responsible gels exhibited 44.49 ± 3.12 % inhibitions of free radicals in DPPH assay. The polymer-drug interactions demonstrated sustained diffusion of methotrexate with non-Fickian diffusion and Korsmeyer-Peppas kinetic model. Overall, co-polymeric network structure was found useful in colon specific drug delivery.


Assuntos
Psyllium , Psyllium/química , Hidrogéis/química , Sistemas de Liberação de Medicamentos , Polímeros/química
3.
RSC Adv ; 12(7): 4081-4093, 2022 Jan 28.
Artigo em Inglês | MEDLINE | ID: mdl-35425464

RESUMO

Recently, dinitrogen (N2) binding and its activation have been achieved by non-metal compounds like intermediate cAAC-borylene as (cAAC)2(B-Dur)2(N2) [cAAC = cyclic alkyl(amino) carbene; Dur = aryl group, 2,3,5,6-tetramethylphenyl; B-Dur = borylene]. It has attracted a lot of scientific attention from different research areas because of its future prospects as a potent species towards the metal free reduction of N2 into ammonia (NH3) under mild conditions. Two (cAAC)(B-Dur) units, each of which possesses six valence electrons around the B-centre, are shown to accept σ-donations from the N2 ligand (B ← N2). Two B-Dur further provide π-backdonations (B → N2) to a central N2 ligand to strengthen the B-N2-B bond, providing maximum stability to the compound (cAAC)2(B-Dur)2(N2) since the summation of each pair wise interaction accounted for the total stabilization energy of the molecule. (cAAC)(B-Dur) unit is isolobal to cAAC-E (E = Si, Ge) fragment. Herein, we report on the stability and bonding of cAAC-E bonded N2-complex (cAAC-E)2(N2) (1-2; Si, Ge) by NBO, QTAIM and EDA-NOCV analyses (EDA-NOCV = energy decomposition analysis coupled with natural orbital for chemical valence; QTAIM = quantum theory of atoms in molecule). Our calculation suggested that syntheses of elusive (cAAC-E)2(N2) (1-2; Si, Ge) species may be possible with cAAC ligands having bulky substitutions adjacent to the CcAAC atom by preventing the homo-dimerization of two (cAAC)(E) units which can lead to the formation of (cAAC-E)2. The formation of E[double bond, length as m-dash]E bond is thermodynamically more favourable (E = Si, Ge) over binding energy of N2 inbetween two cAAC-E units.

4.
J Comput Chem ; 43(11): 757-777, 2022 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-35289411

RESUMO

Binding of dinitrogen (N2 ) to a transition metal center (M) and followed by its activation under milder conditions is no longer impossible; rather, it is routinely studied in laboratories by transition metal complexes. In contrast, binding of N2 by main group elements has been a challenge for decades, until very recently, an exotic cAAC-borylene (cAAC = cyclic alkyl(amino) carbene) species showed similar binding affinity to kinetically inert and non-polar dinitrogen (N2 ) gas under ambient conditions. Since then, N2 binding by short lived borylene species has made a captivating news in different journals for its unusual features and future prospects. Herein, we carried out different types of DFT calculations, including EDA-NOCV analysis of the relevant cAAC-boron-dinitrogen complexes and their precursors, to shed light on the deeper insight of the bonding secret (EDA-NOCV = energy decomposition analysis coupled with natural orbital for chemical valence). The hidden bonding aspects have been uncovered and are presented in details. Additionally, similar calculations have been carried out in comparison with a selected stable dinitrogen bridged-diiron(I) complex. Singlet cAAC ligand is known to be an exotic stable species which, combined with the BAr group, produces an intermediate singlet electron-deficient (cAAC)(BAr) species possessing a high lying HOMO suitable for overlapping with the high lying π*-orbital of N2 via effective π-backdonation. The BN2 interaction energy has been compared with that of the FeN2 bond. Our thorough bonding analysis might answer the unasked questions of experimental chemists about how boron compounds could mimic the transition metal of dinitrogen binding and activation, uncovering hidden bonding aspects. Importantly, Pauling repulsion energy also plays a crucial role and decides the binding efficiency in terms of intrinsic interaction energy between the boron-center and the N2 ligand.

5.
Eur Stroke J ; 6(2): 176-184, 2021 Jun.
Artigo em Inglês | MEDLINE | ID: mdl-34414293

RESUMO

INTRODUCTION: Despite a high burden of stroke, access to rapid brain imaging is limited in many middle- and low-income countries. Previous studies have described the astroglial protein GFAP (glial fibrillary acidic protein) as a biomarker of intracerebral hemorrhage. The aim of this study was to test the diagnostic accuracy of GFAP for ruling out intracranial hemorrhage in a prospective cohort of Indian stroke patients. PATIENTS AND METHODS: This study was conducted in an Indian tertiary hospital (Christian Medical College, Ludhiana). Patients with symptoms suggestive of acute stroke admitted within 12 h of symptom onset were enrolled. Blood samples were collected at hospital admission. Single Molecule Array technology was used for determining serum GFAP concentrations. RESULTS: A total number of 155 patients were included (70 intracranial hemorrhage, 75 ischemic stroke, 10 stroke mimics). GFAP serum concentrations were elevated in intracranial hemorrhage patients compared to ischemic stroke patients [median (interquartile range) 2.36 µg/L (0.61-7.16) vs. 0.18 µg/L (0.11-0.38), p < 0.001]. Stroke mimics patients had a median GFAP serum level of 0.14 µg/L (0.09-0.26). GFAP values below the cut-off of 0.33 µg/L (area under the curve 0.871) ruled out intracranial hemorrhage with a negative predictive value of 89.7%, (at a sensitivity for detecting intracranial hemorrhage of 90.0%). DISCUSSION: The high negative predictive value of a GFAP test system allows ruling out patients with intracranial hemorrhage. CONCLUSION: In settings where immediate brain imaging is not available, this would enable to implement secondary prevention (e.g., aspirin) in suspected ischemic stroke patients as soon as possible.

6.
Opt Express ; 27(17): 24093-24104, 2019 Aug 19.
Artigo em Inglês | MEDLINE | ID: mdl-31510303

RESUMO

We report the first realization of widely tunable continuous-wave (cw) optical parametric oscillator (OPO) based on periodically-poled KTiOPO4 (PPKTP) at room temperature. By exploiting fan-out grating design in a 30-mm PPKTP crystal, and configured in an output-coupled singly-resonant oscillator (OC-SRO) configuration pumped at 532 nm in the green, the OPO provides finely tunable radiation across 741-922 nm in the signal and 1258-1884 nm in the idler, at a fixed temperature of 25 °C. The use of output coupling for the signal wave enables enhancement of OPO extraction efficiency to 30%, providing a maximum total output power of 1.65 W (450 mW of signal at 901 nm and 1.2 W of idler at 1299 nm) for 5.5 W of pump power. The output idler exhibits passive power stability better than 3.2% rms over >2 mins, and the extracted signal exhibits frequency stability of 194 MHz over more than 35 seconds, in excellent beam quality. The OPO performance in pure SRO configuration has also been investigated.

7.
Opt Lett ; 43(10): 2284-2287, 2018 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-29762573

RESUMO

We report the generation of tunable continuous-wave (cw) mid-infrared (mid-IR) radiation across 4608-4694 nm using the new nonlinear material, orientation-patterned gallium phosphide (OP-GaP). By exploiting difference-frequency mixing between a cw Tm-fiber laser and a home-built cw optical parametric oscillator in a 40-mm-long crystal, we have generated up to 43 mW of cw output power, with >30 mW across >95% of the mid-IR tuning range. The output at 4608 nm exhibits high beam quality with a passive power stability of 2.5% rms over 1.5 min. The temperature acceptance bandwidth of the OP-GaP crystal has been measured and compared with theory. The performance of the mid-IR source at high pump powers and polarization-dependent transmission in OP-GaP has been investigated.

8.
Molecules ; 23(5)2018 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-29757989

RESUMO

A new class of compounds comprising two series of chalcones with 2,2,2-trifluoroethoxy group and 2-fluoroethoxy groups were synthesized and screened for in vitro antiplasmodial activity against Plasmodium falciparum (3D7) using the [³H] hypoxanthine incorporation inhibition assay. Chalcones with 2,2,2-trifluoroethoxy groups substituted on the p- and m-positions of the 1-phenyl ring showed weak antiplasmodial activity, while compounds substituted on the o-position of the 1-phenyl ring displayed enhanced antiplasmodial activity, thus indicating that 2,2,2-trifluoroethoxy groups on the 1-phenyl ring of chalcones show position-dependent antiplasmodial activity. Of the 34 compounds synthesized, chalcones 3a and 3f exhibited significant inhibitory effects, with IC50 values of 3.0 µg/mL and 2.2 µg/mL, respectively. Moreover, these compounds 3a and 3f showed profound antiplasmodial activity in combination with artemisinin in vitro. The most active molecules, 3a, and 3f, were further assessed for their cytotoxicity towards mammalian Vero cells and the selectivity index (SI) values are 8.6, and 8.2 respectively, being considered non-toxic. We also studied the antiplasmodial activity of 2-fluoroethoxychalcones to discern the effect of the number of fluorine atoms in the fluoroethoxy group. Our results showed that chalcones with 2-fluoroethoxy group on the 1-phenyl ring exhibited more enhanced inhibitory effects on the growth of parasites than their trifluoro analogues, which reveals that monofluoroethoxy group is generally more effective than trifluoroethoxy group in the inhibition of parasite growth. Thus o-2,2,2-trifluoroethoxychalcones (Series 3) and 2-fluoroethoxychalcones may serve as good antiplasmodial candidates for future further development.


Assuntos
Antimaláricos/síntese química , Antimaláricos/farmacologia , Chalconas/síntese química , Chalconas/farmacologia , Plasmodium falciparum/efeitos dos fármacos , Animais , Antimaláricos/química , Chalconas/química , Técnicas de Química Sintética , Chlorocebus aethiops , Eritrócitos/efeitos dos fármacos , Eritrócitos/parasitologia , Concentração Inibidora 50 , Malária Falciparum/tratamento farmacológico , Malária Falciparum/parasitologia , Testes de Sensibilidade Parasitária , Células Vero
9.
Opt Lett ; 42(13): 2635-2638, 2017 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-28957303

RESUMO

We report a high-power, single-frequency, green-pumped continuous-wave optical parametric oscillator (OPO) capable of providing rapid and continuous tuning across a wide spectral range in the near-infrared at room temperature. By exploiting the nonlinear crystal of MgO:sPPLT in a fan-out grating design pumped at 532 nm in the green, the OPO can be tuned continuously across 1097-2100 nm in the idler, with corresponding signal tuning over 712-1033 nm using simple mechanical translation of the crystal at fixed temperature. The device can deliver hundreds of milliwatts of idler power across the complete tuning range, with as much as 2.2 W at 1097 nm for 9 W of input pump power at 77% pump depletion. The passive power stability of the generated idler at 1110 nm, measured at 6.8 W of pump power, is better than 1% rms over 30 min. The signal frequency stability, measured at 837 nm, is 518 MHz over 2 min, with an instantaneous linewidth of 6.9 MHz, in high beam quality.

10.
Opt Lett ; 42(11): 2193-2196, 2017 Jun 01.
Artigo em Inglês | MEDLINE | ID: mdl-28569879

RESUMO

We report a tunable, single-pass, pulsed nanosecond difference-frequency generation (DFG) source based on the new semiconductor nonlinear material, orientation-patterned gallium phosphide (OP-GaP). The DFG source is realized by mixing the output signal of a nanosecond OPO tunable over 1723-1827 nm with the input pump pulses of the same OPO at 1064 nm in an OP-GaP crystal, resulting in tunable generation over 233 nm in the mid-infrared from 2548 to 2781 nm. Using a 40-mm-long crystal, we have produced ∼14 mW of average DFG output power at 2719 nm for a pump power of 5 W and signal power of 1 W at 80 kHz repetition rate. To the best of our knowledge, this is the first single-pass nanosecond DFG source based on OP-GaP. The DFG output beam has a TEM00 spatial mode profile and exhibits passive power stability better than 1.7% rms over 1.4 h at 2774 nm, compared to 1.6% and 0.1% rms for the signal and pump, respectively. The OP-GaP crystal is recorded to have a temperature acceptance bandwidth of 17.7°C.

11.
Opt Lett ; 41(20): 4799-4802, 2016 Oct 15.
Artigo em Inglês | MEDLINE | ID: mdl-28005896

RESUMO

We report a compact, fiber-laser-based, high-repetition-rate picosecond source for the ultraviolet (UV), providing multi-tens of milliwatt of average power across 329-348 nm. The source is based on internal sum-frequency-generation (SFG) in a singly resonant optical parametric oscillator (OPO), synchronously pumped at 532 nm by the second harmonic of a picosecond Yb-fiber laser at 80 MHz repetition rate. Using a 30-mm-long single-grating MgO:sPPLT crystal for the OPO and a 5-mm-long BiB3O6 crystal for intracavity SFG, we generate up to 115 mW of average UV power at 339.9 nm, with >50 mW over 73% of the tuning range, for 1.6 W of input pump power. The UV output exhibits a passive rms power stability of ∼2.9% rms over 1 min and 6.5% rms over 2 h in high beam quality. Angular acceptance bandwidth and cavity detuning effects have also been studied.

12.
Opt Lett ; 41(12): 2715-8, 2016 Jun 15.
Artigo em Inglês | MEDLINE | ID: mdl-27304271

RESUMO

We report on the generation of ultrafast vortex beams in the deep ultraviolet (DUV) wavelength range at 266 nm, for the first time to our knowledge. Using a Yb-fiber-based green source in combination with two spiral phase plates of orders 1 and 2, we were able to generate picosecond Laguerre-Gaussian (LG) beams at 532 nm. Subsequently, these LG beams were frequency doubled by single-pass, second-harmonic generation in a 10 mm-long ß-BaB2O4 crystal to generate ultrafast vortex beams at 266 nm with a vortex order as high as 12, providing up to 383 mW of DUV power at a single-pass, green-to-DUV conversion efficiency of 5.2%. The generated picosecond UV vortex beam has a spectral width of 1.02 nm with a passive power stability better than 1.2% rms over >1.5 h.

13.
Opt Express ; 24(8): 8763-75, 2016 Apr 18.
Artigo em Inglês | MEDLINE | ID: mdl-27137310

RESUMO

We report the implementation of a compact cascaded multicrystal scheme based on birefringent crystals in critical phase-matching, for the generation of continuous-wave (cw) radiation in the deep ultraviolet (UV). The approach comprises a cascade of 4 single-pass second-harmonic-generation (SHG) stages in ß-BaB2O4 (BBO) pumped by a single-frequency cw green source at 532 nm. A deep-UV cw output power of 37.7 mW at 266 nm has been obtained with a high passive power stability of 0.12% rms over more than 4 hours. Characterization and optimization of the system in each stage has been systematically performed. Angular phase-matching acceptance bandwidth under tight focusing in BBO, and spectral properties of the deep-UV radiation, have been studied. Theoretical calculations for SHG in the cascaded scheme based on birefringent phase-matching have been performed, and enhancement in UV power compared to single-stage single-pass scheme are studied. Theoretical comparison of BBO with other potential crystals for deep-UV generation in cascaded multicrystal scheme is also presented.

14.
Opt Lett ; 39(23): 6751-4, 2014 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-25490669

RESUMO

We report a continuous-wave (cw) source of tunable mid-infrared radiation providing tens of milliwatt of output power in the 6460-7517 nm spectral range. The source is based on difference-frequency generation (DFG) in orientation-patterned (OP)-GaAs pumped by a Tm-fiber laser at 2010 nm and a 1064 nm-Yb-fiber-pumped cw optical parametric oscillator. Using a 25.7-mm-long OP-GaAs crystal, we have generated up to 51.1 mW of output power at 6790 nm, with >40 mW and >20 mW across 32% and 80% of the mid-infrared tuning range, respectively, which is to the best of our knowledge the highest tunable cw power generated in OP-GaAs in this spectral range. The DFG output at maximum power exhibits passive power stability better than 2.3% rms over more than 1 h and a frequency stability of 1.8 GHz over more than 1 min, in high spatial beam quality. The system and crystal performance at high pump powers have been studied.

15.
Chemistry ; 20(44): 14218-25, 2014 Oct 27.
Artigo em Inglês | MEDLINE | ID: mdl-25236851

RESUMO

We report an unprecedented BrettPhos ligand supported Pd-catalyzed CO bond-forming reaction of activated aryl halides with primary fluoroalkyl alcohols. We demonstrate that the Phosphine ligand (BrettPhos) possesses the property of altering the mechanistic pathway of reductive elimination from nucleophile to nucleophile. The Pd/BrettPhos catalyst system facilitates the reductive elimination of the oxygen nucleophile through an electronic pathway.

16.
Opt Lett ; 38(23): 5114-7, 2013 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-24281523

RESUMO

We report stable continuous-wave (CW) ultraviolet (UV) generation at 354.7 nm using single-pass sum-frequency-generation (SFG) of a CW Yb-fiber laser at 1064 nm in the nonlinear crystal, BiB3O6. The 532 nm radiation is obtained by single-pass second-harmonic generation of the Yb-fiber laser in a 30-mm-long MgO:sPPLT crystal. Using a 10-mm-long BiB3O6 crystal for SFG, with a measured angular acceptance bandwidth of 0.57 mrad, we generate as much as 68 mW of CW single-frequency UV radiation with a passive power stability better than 3.2% rms over 2 h and frequency stability better than 436 MHz over 2.5 h. The UV output beam has a TEM00 spatial profile with M(x)(2)<1.6 and M(y)(2)<1.8.

17.
Opt Express ; 21(20): 23365-75, 2013 Oct 07.
Artigo em Inglês | MEDLINE | ID: mdl-24104250

RESUMO

We present results on direct mode-locking of a doubly-resonant optical parametric oscillator (DRO) using an electro-optic phase modulator with low resonant frequency of 80 MHz as the single mode-locking element. Pumped by a cw laser at 532 nm and based on MgO:sPPLT as the nonlinear material, the DRO generates 533 ps pulses at 80 MHz and 471 ps pulses at 160 MHz. Stable train of mode-locked pulses is obtained at a modulation depth of 1.83 radians when the modulation frequency is precisely tuned and the cavity length is carefully adjusted. The effects of frequency detuning, modulation depth, input laser pump power, crystal temperature and position of modulator inside the cavity, on pulse duration and repetition rate have been studied. Operating at degeneracy, under mode-locked condition, the signal-idler spectrum exhibits a bandwidth of ~31 nm, and the spectrum has been investigated for different phase-matching temperatures. Mode-locked operation has been confirmed by second-harmonic-generation of the DRO output in a ß-BaB2O4 crystal, where a 4 times enhancement in green power is observed compared to cw operation.

18.
Opt Express ; 21(21): 24829-36, 2013 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-24150326

RESUMO

We report a continuous-wave (cw) source of tunable radiation across 333-345 nm in the ultraviolet (UV) using bismuth triborate, BiB3O6 (BIBO) as the nonlinear gain material. The source is based on internal sum-frequency-generation (SFG) in a cw singly-resonant optical parametric oscillator (OPO) pumped at 532 nm. The compact tunable source employs a 30-mm-long MgO:sPPLT crystal as the OPO gain medium and a 5-mm-long BIBO crystal for intracavity SFG of the signal and pump, providing up to 21.6 mW of UV power at 339.7 nm, with >15 mW over 64% of the SFG tuning range. The cw OPO is also tunable across 1158-1312 nm in the idler, delivering as much as 1.7 W at 1247 nm, with >1W over 65% of the tuning range. The UV output at maximum power exhibits passive power stability better than 3.4% rms and frequency stability of 193 GHz over more than one minute.

19.
Opt Lett ; 37(24): 5049-51, 2012 Dec 15.
Artigo em Inglês | MEDLINE | ID: mdl-23258001

RESUMO

We report a high-power, single-frequency, continuous-wave (cw) source tunable across 775-807 nm in the near-infrared, based on internal second harmonic generation (SHG) of a cw singly-resonant optical parametric oscillator (OPO) pumped by a Yb-fiber laser. The compact, all-periodically-poled source employs a 48-mm-long, multigrating MgO doped periodically poled lithium niobate (MgO:PPLN) crystal for the OPO and a 30-mm-long, fan-out grating MgO-doped stoichiometric periodically poled lithium tantalate (MgO:sPPLT) crystal for intracavity SHG, providing as much as 3.7 W of near-infrared power at 793 nm, together with 4 W of idler power at 3232 nm, at an overall extraction efficiency of 28%. Further, the cw OPO is tunable across 3125-3396 nm in the idler, providing as much as 4.3 W at 3133 nm with >3.8 W over 77% of the tuning range together with >3 W of near-infrared power across 56% of SHG tuning range, in high-spatial beam-quality with M2<1.4. The SHG output has an instantaneous linewidth of 8.5 MHz and exhibits a passive power stability better than 3.5% rms over more than 1 min.


Assuntos
Amplificadores Eletrônicos , Tecnologia de Fibra Óptica/instrumentação , Lasers , Oscilometria/instrumentação , Transferência de Energia , Desenho de Equipamento , Análise de Falha de Equipamento , Raios Infravermelhos
20.
Opt Lett ; 37(18): 3909-11, 2012 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-23041900

RESUMO

We report an actively mode-locked continuous-wave (cw) optical parametric oscillator in singly resonant oscillator (SRO) configuration, generating stable 230 ps pulses at 80 MHz repetition rate. The idler-resonant cw SRO, configured in standing-wave cavity, is based on MgO:sPPLT as the nonlinear gain material and pumped at 532 nm. Mode-locking is achieved by direct deployment of an intracavity phase modulator close to one of the SRO cavity end mirrors. The effects of modulation depth and modulation frequency on mode-locked pulse duration and repetition rate are investigated for both idler and signal pulses. Mode-locking is further confirmed by enhancement of single-pass second-harmonic generation of SRO output in the crystal of ß-BaB(2)O(4).

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