«Chaînes Aimants» et «Molécules Aimants» dans les Oxydes. GDR MCM2 & MEETICC Strasbourg, 5 6 octobre 2017
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1 «Chaînes Aimants» et «Molécules Aimants» dans les Oxydes MCM2 MEETICC GDR MCM2 & MEETICC Strasbourg, 5 6 octobre 2017 «Propriétés magnétiques & électroniques : échelles de temps et d espace» Can oxides be complementary to molecular compounds in the investigation of the «0D & 1D nanomagnets related to blocking effects»? Present report Sr 4 CoMn 2 O 9 Seikh et al. (2017) Previous reports in inorganic materials Dy 2 Ti 2 O 7 Snyder et al. (2003) Ca 3 Co 2 O 6 Hardy et al. (2004) Ca 3 CoMnO 6 Choi et al. (2008) BaCo 2 (As 3 O 6 ) 2 2(H 2 O) David et al. (2013)
2 SINGLE ION AND SINGLE CHAIN MAGNETISM IN TRIANGULAR SPIN CHAIN OXIDES V. Hardy 1, M. Seikh 2, V. Caignaert 1, O. Perez 1, and B. Raveau 1 1 Laboratoire CRISMAT, UMR 6508, CNRS/ENSICAEN/UNICAEN, Caen, France 2 Department of Chemistry, Visva-Bharati University, Santiniketan, West Bengal, India CRISMAT Visva-Bharati 0D 1D SIM (Single Ion Magnet) : individual spins SMM (Single Molecule Magnet) : clusters SCM (Single Chain Magnet) : chains
3 SIM (Single Ion Magnet) SMM (Single Molecule Magnet) SCM (Single Chain Magnet) Magnet M H Usually : «Magnet» Long Range Ordering (LRO) below a T C µm Magnetostatics / Domain boundaries Here: «Magnet» Blocking of the spins (without LRO) below a T B (f) Spin dynamics / Individual reversals Anisotropy Barrier nm Blocking : = 0 exp( / T) > Exp. Time log t exp 1/T
4 Spin reversal mechanisms 0D SIM (Single Ion Magnet) SMM (Single Molecule l l Magnet) 0 0 1D SCM (Single Chain Magnet) 2 2 2JS 2 +S 1 S+1 +S S Thermally Activated = D S 2 (D: anisotropy parameter) Quantum Tunneling of Magnetization (QTM) TA QTM Thermally Activated = DS 2 + 8JS 2
![Single Molecule Magnet [Mn 12 O 12 (CH 3 CO 2 ) 16 (H 2 O) 4 ].2CH 3 CO 2 H.4H 2 O Mn 3+ Mn 4+ «Mn 12» Sessoli et al.](/docs-images/88/115502822/images/5-0.jpg "Nature 365, 141 (1993) Single Chain Magnet [Co(hfac) 2 NITPhOMe] hfac =hexafluoroacetylacetonate NITPhOMe=4 methoxy phenyl 4 methoxy phenyl 4,4,5,5,")
5 Single Molecule Magnet [Mn 12 O 12 (CH 3 CO 2 ) 16 (H 2 O) 4 ].2CH 3 CO 2 H.4H 2 O Mn 3+ Mn 4+ «Mn 12» Sessoli et al. Nature 365, 141 (1993) Single Chain Magnet [Co(hfac) 2 NITPhOMe] hfac =hexafluoroacetylacetonate NITPhOMe=4 methoxy phenyl 4 methoxy phenyl 4,4,5,5, tetramethylimidazoline 1 oxyl 3 oxide 455 tetramethylimidazoline 1 oxyl 3 oxide Co 2+ DS 2 (D+8J)S 2 Easy axis Easy axis+fm like «Co(hfac)» Caneschi et al. Angew. Chem. Int. Ed. 40, 1760 (2001) M(H) loops at low T M(H) loops at low T 0 exp( / T ) exp( / T ) K sec K 11 sec Novak et al., JMMM 294, 133 (2005) Novak et al., JMMM 294, 133 (2005)
6 Sr 4 CoMn 2 O 9 Belongs to the family of the 2D perovskite related oxides Spin chains Triangular lattice c c [Trigonal Prism] [Octahedra] TP O O Co 2+ Mn 4+ Mn 4+ Sr 2+ «1D» + «Geometrical Frustration» J F J AF?
7 Sr 4 CoMn 2 O 9 : magnetic features Easy axis anisotropy 0 2 Co 2+ (3d 7 ) in Trigonal Prism z TP O O Co 2+ Mn 4+ Mn 4+ Co 2+ CEF + SO GS doublet with g =8 9 Ising like anisotropy GS 2 z ( Co TP ) 4 4. B ) 5 Abragam and B. Bleaney (1970). F. Lloret et al., Inorg. Chim. Acta. 361, 3432 (2008). S. Gómez Coca et al., Coord. Chem. Rev , 290, 379 (2015).
8 Sr 4 CoMn 2 O 9 : magnetic features (at least) 4 competing intrachain interactions J 1 J intra (nn & nnn) expected to be AF in this family J 2 TP Co 2+ J «Geometrical Frustration» 4 OO Mn 4+ (not only interchain) Mn 4+ J 3 but also intrachain?
9 Sr 4 CoMn 2 O 9 : magnetic features Intrachain coupling: trend towards ferrimagnetism J 1 E min (Mn 4+ Mn 4+ Co 2+ ) = () if (J 2 J 3 ) < J 4 < (J 2 +J 3 ) J 2 Sr 4 Mn 2 NiO 9 : El Abed et al., JSSC 2002 Ca 3 CoMnO 6 : Zhang et al., PRB 2009 J 1 35 K J 2 26 K ( H = + 2k B J S S ) J 3 27 K Co 2+ J 4 Mn 4+ J 3 Mn 4+ J 3 E min () 1 K < J 4 < 53 K (very likely)
10 Sr 4 CoMn 2 O 9 : magnetic features Interchain coupling : weak and frustrated Sr 2+ d* Small J* Sr 2+ large d* (5.53 Å) Sr 2+ weak coupling (Sr 2+ ) Sr 2+ Sr 2+ J* Sr 2+ (AF interchain coupling) Strong Geometrical Frustration J*is AF Ising chains
11 Sr 4 CoMn 2 O 9 Ceramic samples Ac susceptibility ' (emu/m mol Oe) Hz 10 2 Hz 10 3 Hz 10 4 Hz T p / T p log f 0.12 [Boulahya et al. (2003)] Another relaxation mechanism. Heat capacity -1 ) K -1 mol No signature of LRO (Long Range Ordering) C p (J
12 Cole Cole Generalization of the Debye model with a distribution of relaxation times around c characterized by a parameter (0 < < 1) 0 ( T ) ( T ) (, T ) ( T ) (1 ) 1 i c ( T ) 0 : isothermal susceptibility : adiabatic susceptibility : width of the distribution 4 1 (a.u..) '' 2K 3 3K 2 4K 2 5K 6K 7K 1 8K 9K 10K ' (a.u.) Coexistence of 2 relaxation processes ( )
13 Spin relaxation time c (T) Peak in (T, f) (1 ) ( ) cos( / 2) ''(, ) 0 T x f T Max for x 2πf τ ( T ) 1 2(1 ) (1 ) 1 2 sin( / 2) c x x 0.05 c (T peak )=1/(2f) 1 c (T)=1/(2f peak ) '' (emu u/mol Oe e) Hz /mol Oe) '' (emu log log frequency (Hz) 2K 10K 8K 6K 4K /T Max (T) 2f c 1 Max (f) 2f c = 1 1/T
14 Sr 4 CoMn 2 O 9 (sec) c vs. T /T (K -1 ) 2 vs. f vs. f ' (e emu/mol Oe) Hz Hz c (sec) /T (K -1 ) 1 0 exp( / T ) s K SCM? (Single Chain i Magnet)
15 The basic ingredients for SCM : 1 Easy axis axis anisotropy 2 Chains with a net magnetization 3 Free (uncoupled) chains Co 2+ Mn 4+ Mn z
16 Sr 4 CoMn 2 O SCM sec) c ( Co 2+? Mn 4+ Mn /T (K -1 ) LowTbehavior Quantum Tunneling? SMM / SIM? SIM of Co 2+? SIM of Co? in TP JACS (2015)
17 Two relaxation mechanisms SCM Single Chain Magnet Co 2+ Mn 4+ Mn 4+ SIM Single Ion Magnet
18 Sr 4 CoMn 2 O 9 c (sec) 10-1 SCM (Single Chain Magnet) (Single Ion Magnet) SIM Co 2+ Mn 4+ Mn /T (K -1 ) Dynamical responses in zero field well compatible with SCM & SIM SCM : = 0 exp(/t) sec & 167 K SIM : 1 = [ 0 exp(/t)] 1 + [r/t n ] 1 + [ QTM ] sec & 40 K but what about the M(H)?
19 Sr 4 CoMn 2 O 9 : dc magnetization M (µ B /f.u.) M rem H coer T =2K µ 0 H (T) 0 M(H) loop while no (detected) LRO
20 Sr 4 CoMn 2 O 9 : dc magnetization «Saturation» magnetization as expected M (µ B /f..u.) M rem H coer M (µ B /f.u.) T = 2 K GS 2 (1/ 2) z ( Co TP ) µ 0 H (T) -1.0 T = 2 K Remanent magnetization is «robust» µ 0 H (T) µ B /Co) M rem ( days T = 2 K 150 years time (sec)
21 M rem (µ B /f f.u.) M rem : 0 9T 0 Sr 4 CoMn 2 O 9 : dc magnetization ' (emu/m mol Oe) Hz 10 2 Hz 10 3 Hz Hz dc (em mu/mol Oe e) FCC 0.2 T b 0.1 T (sec) K «magnet» SCM SIM ZFC /T (K -1 )
22 Sr 4 x Ca x CoMn 2 O 9 (Sr,Ca) IR (Sr 2+ ) 1.26 Å IR (Ca 2+ ) 1.12 Å Chemical pressure effects x=2 Sr 2 Ca 2 CoMn 2 O 9
23 x=0 : Sr 4 CoMn 2 O 9 & x=2 : Sr 2 Ca 2 CoMn 2 O 9 ' (em mu/mol Oe)0.3 x= Hz 0.2 LRO 0.1 x= C K -1 mo ol -1 p (J ) x=0 25 x= LRO ) mu/mol M (em sp pont 3 x=2 LRO x= K 5K NPD x=2
24 x=2 : Sr 2 Ca 2 CoMn 2 O K 5K NPD x=2 ' (emu/m mol Oe) x=0 x=2 LRO Ising chains Triangular lattice Partially Disordered Antiferromagnet (PDA) M. Mekata, J. Phys. Soc. Jpn. 42, 76 (1977) + + Ferrimagnetic UP I + Ferrimagnetic DOWN + I Incoherent (zero net magnetization) Observed magnetic LRO «consistent with» PDA
25 '' (emu/m mol Oe) x=2 x=0 x=0 : Sr 4 CoMn 2 O 9 & x=2 : Sr 2 Ca 2 CoMn 2 O Hz (sec) 10-1 LRO SCM x= x=2 SIM 10-3 x 2 SIM 10-4 SIM '' (em mu/mol Oe) Hz x= x= /T (K -1 ) Sr 4CoMn 2O 9 Sr 2Ca 2CoMn 2O 9 SCM LRO SIM SIM
26 Crossover vs. x : Sr 4 x Ca x CoMn 2 O LRO Maxima in (T) T(K) SCM SIM Filled symbols : 10 2 Hz Empty symbols : 10 4 Hz x SIM (Single Ion Magnet) SMM (Single Molecule Magnet) SCM (Single Chain Magnet) LRO (Long Range Ordering) «Moléculaires» Sr 4 x Ca x CoMn 2 O 9 SIM SMM LRO SCM
27 C p : Sr 4 x Ca x CoMn 2 O x = x = 2 C/T (JK -2 mol -1 ) H = 0 T H = 9 T C/T (JK -2 mol -1 ) H = 0 T H = 9 T x = 0 x = C/T (JK -2 mol -1 ) C/T (JK -2 mol -1 ) 0 T 1 T 0 T 1 T 3 T T 5 T 5 T OK with SCM? 7 T OK with SIM? 7 T 9 T 9 T
28 Signature of blocking on the Cp of SMM/SCM? SMM Fominaya et al., PRB 59, 519 (1999) 2 2 C bi 2 Cbi Cuni C( T, texp) Cuni C +S S 1 t exp C uni ep exp /T T blocking C uni C bi +S S T SCM? C mag / R D Ising Insensitive to «blocking»? T/J
29 SMM Gomes et al., PRB 57, 5021 (1998) Mn 12 Ac Mettes et al., PRB 64, (2001) T B T B 0.3T 0T 1D Ising chains made Bhattacharjee et al., Polyhedron 20, 1607 (2001) of S=9 Mn 4 clusters 0T & 9T [Mn 4 4( (hmp) 6 R 2 ](ClO 4 4) 2 A : R=OAc B : R=Cl T B? 0T
30 C p : Sr 4 x Ca x CoMn 2 O x = 0 x = 2 C/T (JK -2 mol -1 ) C/T (JK -2 mol -1 ) 0.3 dc (emu u/mol Oe) H = 0 T x = 0 x = T b ZFC 0.1 T dc (emu/m mol Oe) H = 0 T? T b ZFC 0.1 T
31 SINGLE ION AND SINGLE CHAIN MAGNETISM IN TRIANGULAR SPIN CHAIN OXIDES V. Hardy, V. Caignaert, O. Perez, B. Raveau CRISMAT, Caen M. Seikh Visva Bharati University, Santiniketan c (sec) /T (K -1 ) M (µ B /f.u.) T = 2 K µ 0 H (T) T(K) SCM LRO SIM x 1 ) C/T (JK -2 mol T 9 T To be done : Planned tasks : Single crystals, NPD, INS, High fields, Other 3d combinations, etc Collaborations with people of «Molecular Magnetism»! We hope that oxides might be complementary to molecular compounds in the investigation of the «0D & 1D nanomagnets related to blocking effects» Thank you GDR MCM2 & MEETICC Strasbourg, 5 6 octobre 2017
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