Yang-Yuan Chen Low temperature and nanomaterial labatory Institute of Physics, Academia Sinica

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1 Yang-Yuan Chen Low temperature and nanomaterial labatory Institute of Physics, Academia Sinica

2 Introduction: 1. Metal Nanoclusters 2. Semiconducting Nanoclusters 3. Rare Gas and Molecular Clusters 4. Methods of Synthesis

3 Nanoparticles size? ~ nm Criterion: Critical length or characteristic length 1. Thermal diffusion length 2. Scattering length ( mean free path) 3. Coherence length 4. Energy level spacing >> thermal energy KT 5. Surface effect 6. other

4 0.1 atom Microscopic ( ) Mesoscopic ( ) Macroscopic ( )

5 Virus ~10 nm~100 nm blood cell 200~300 nm bacteria 200~600 nm

6 Energy

7

8 Surface effect With FCC structure

9 4.2.1 Magic numbers and structure No. of electrons for an atom: electronic magic numbers example He2: 1S 2 Ne10: 1S 2,2S 2, 2P 6 Ar 18: 1S 2,2S 2, 2P 6,3S 2, 3P 6, Kr 36: 1S 2,2S 2, 2P 6,3S 2, 3P 6, 3d No. of atoms for a nanoparticles Structural magic number The jellium model P75

10

11 (Excimer Laser Ablation ELA )( 2003/3) ( 1993/1)

12

13 4.2.2 Theoretical Modeling of Nanoparticles Electronic magic numbers: the total mumber of electrons on the superatom when the top level is filled The jellium model P75 Structural magic number:cluster has a size in which all the energy levels are filled

14 Theoretical calculation:cluster as molecular Molecular orbital theory P78 Density functional theory P78 Find the structure and geometry with the lowest energy

15 4.2.3 Geometric Structure

16 Size dependent structure of Indium nanoparticles Face-centered tetragonal Face-centered cubic

17 Magic number C 20, C 24, C 28, C 32, C 36, C 50, C 60, C 70

18 Ta (110) Tetragonal count(arb. unit) 14nm 16nm 19nm (002)* (410)* (411)* (331)* (200) (631)* (413)* (720)* (211) (820)* (220) 21nm bulk Cubic Size dependence of phase compositions 2 θ (d e g re e ) X ray spectra of Ta

19 lattice constant of Ta cubic-ta Ta bulk Lattice constant(a) bulk Size(nm) c/a Size(nm) Ta - Tetragonal Lattice constant(a) o a c Lattice constant(a) o Size(nm)

20 4.2.4 Electronic Structure Bulk 100 atoms 3 atoms Quantum Size Effect : Energy level spacing >> K B T Light-induced transitions between these levels determines the color

21 Light-induced transition between these levels determines the color of the materials

22 UV photo-electron spectroscopy

23 4.2.5 Reactivity

24 4.2.6 Fluctuations?

25 4.2.7 Magnetic cluster Magnetized cluster Nonmagnetic- magnetic transition Superparamagnetism: 1. Orbital magnetic moment 2. Electron spin 3. Levels filled with an even number of electrons net magnetic moment=0 4. Transition ion atoms: Fe, Mn, Co with partially filled inner d-orbital levels- net magnetic moment Parrel align Ferromagnetic 5 Ferromagnetic cluster with DC field superparamagnetism

26 Superparamagnetism

27 Single domain

28 Superparamagnetism Particles with net moment(ferromagnetic particles with moment,tc is high) Mono-domain when d < 100 nm Fluctuation of the magnetic moment like in a paramagnet Moment dependent on particle volume

29 FeSi 2 DC FC 2 ZFC 1 1. The temperature of peak value of χ in ZFC is defined as the Blocking temperature T B 2. χ of ZFC and χ of FC deviate at T B 3. Above T B, χ of ZFC and χ of FC are overlap.

30 Blocking Temperature k B is the Boltzmann constant K is the anisotropic constant V is the volume of nanoparticle

31 M-H M (emu/g) K 5K H/T (G/K) 1. T< T B Hysteresis appears in M-H. Due to thermal energy is less than the interactions among particles 2. T> T B No hysteresis appears in M-H. Since thermal energy is larger than the interactions among particles FeSi 2 40nm particles T B =20 K

32 Nonmagnetic- magnetic transition Rh

33 4.2.8 Bulk to Nanotransition Gold melting point

34 4.3 Semiconducting Nanoparticles Optical Properties blue shift as size is reduced Due to band gap Exciton: bound electron-hole pair,produced by a photon having hv> gap Hydrogen-like: energy level spacing Light-induced transition

35 Hydrogen-like: energy level spacing Light-induced transition

36 What happens when the size of nanoparticles becomes smaller than to the radius of the orbit of exciton? Weak-confinement size d> radius of electron-hole pair: blue shift Strong-confinement size d< radius of electron-hole pair: Motion of the electron and the hole become independent, the exciton does not exist

37 Absorption edge, band gap exciton

38 5. Size dependence properties of quantum dots CdSe surface charge density absorbance A.U ~ 5 nm ~ 4 nm ~ 3 nm Intensity (arb units) nm 4 nm 5 nm Bulk Wavelength (nm) θ (degree)

39 4.3.2 Photofragmentation Si or Ge can undergo fragmentation under laser light Dissociate!

40 4.3.3 Coulombic Explosion F=e 2 /r2

41

42 4.4 Rare Gas and Molecular Clusters Xenon clusters are formed by adiabatic expansion of a supersonic jet of the gas through a small capillary into a vacuum. Xenon Lennard-Jones potential for calculation structure Repulsion of coulombic electronic core Dipole attractive potential

43 4.4.2 Superfluid Clusters By supersonic free-jet expansion He4 : N=7,10,14,23,30 He3: N+ 7,10,14,21,30 Superfluidity: He N=64,128 Fermion has half-integer spin Boson has integer spin

44

45 superfluid When T= 2.2 K lambda point He4 becomes a superfluid, its viscosit drops to zero

46

47 P. Sindzingre PRL 63,1061(1989)

48 At ambient condition 80% of water moleculars Are bounded into clusters

49 4.5 Method of Synthesis 1. RF Plasma 2. Chemical Methods 3. Thermolysis 4. Pulsed Laser Methods

50 4.5.1 RF Plasma

51 4.5.2 Chemical Method Reducing agents Molybdenum

52 Thermolysis(Thermal LiN 3 -> Li decomposition)

53 Electron paramagnetic resorance (EPR) EPR measures the energy absorbed when electromagnetic radiation such as microwave induces a transition between the spin states m s split by a DC magnetic field. m s

54

55 4.5.4 Pulsed Laser Method Silver nitrate+ reducing agent -----> Silver nanoparticle heating

56 Laser Ablation

57 Laser Ablation

58 1. Quantum size effects on the competition between Kondo interaction and magnetic order in 0-D. 8 80A & Bulk CeAl 2 C/T J/mol -1 K A T N T(K) Bulk Conclusion: In 80A -CeAl 2, magnetic ordering completely disappears and the γ reaches 9500 mj/mol Ce K 2. Unsolved problems: In nanoparticle, only 0.7 Mole Ce 3+ left, Is the 0.3 mol non-magnetic Ce really on the surface? or it is just a coincidence.

59 Size dependence of Kondo effects in CePt 2 nanoparticles 5nm (2,2,0) 4 CePt 2 CKondo (0.56 mol Ce, T K =4.6 K) 2 bulk (2,2,2) nm C Kondo (0.58 mol Ce, T K =4.4 K) CePt 2 3.8nm 22nm nm TEM of nanoparticles (220) (311) (222) (400) (331) bulk (2,2,2) (422) (511) 5nm 2θ(degree) (440) X-ray spectra (2,2,0) (531) (620) (533) (622) (444) C(J/mol K) nm 3.8nm C Kondo (0.65 mol Ce, T K =3.4 K) C Kondo (0.71 mol Ce, T K =100 K) T(K) Specific heat of CePt2

60 4.6 Conclusion

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