Isotope Geochemistry Provides fundamental observational constraints on Earth and solar system processes through time A few examples:

Quantitative constraints on 1. Timing of age of solar system formation 2. Formation of the Earth 3. Genesis of terrestrial units: continents, ocean, mantle, core 4. Climate variability over Earth history What has isotope geochemistry done for you lately? 5. Quantitative timescales a. Hominid evolution b. Landscape evolution Ice Sheet Retreat c. 6. Cultural evolution: 14C dating

Isotope Geochemistry Provides fundamental observational constraints on Earth and solar system processes through time A few examples: Quantitative constraints on 1. Timing or age of solar system formation 2. Formation of the Earth 3. Genesis of terrestrial units: continents, ocean, mantle, core 4. Climate variability over Earth history 5. Quantitative timescales a. Hominid evolution b. Landscape evolution Ice Sheet Retreat 6. Cultural evolution: 14C dating

Quantify the antiquity of our solar system:

238U

! 206Pb 235U ! 207Pb

knowledge of relative decay kinetics linear correlation between systems (i.e., meteorites and Earth) 4.55x109 years

Questions: ! What physics is involved? ! What chemistry is involved? ! What assumptions?

Patterson (1956)

Origin of our moon:

Terrestrial isotopic Fractionation Line ! Common correlation between 17O/16O ratios and 18O/16O ratios measured in lunar rocks and Earth rocks Common source ! planetary impact formed the moon What chemistry/physics is behind this logic?

Earth

Wiechert et al., 2001 after Clayton & Mayeda, 1975

Evolution of Earths mantle and crust:

147Sm

! 143Nd

Constraints on: ! Large scale chemical differentiation in mantle ! Timescales ! Models of Earth evolution

DePaolo, 1988

Isotopic proxy records of long-term global climate variability:

Global climate records benthic Foraminifera

Questions: ! How do observable 18O/16O ratios relate to temperature? ! What chemistry/physics is involved? ! What assumptions are involved?

A W

Isotopic proxy records of (pre-industrial) global climate variability:

18O/ 16O of carbonate Antartic Vostok iceis core: function

of: temperature and 18O/16O of water ! global ice volume Epstein (1953) D/H ratio in ice Temp
18O/16O

ratio in carbonate sediments 800 600 400 200 0

Age (103 years before present)

Augustin et al., 2004

Isotopic proxy records of (pre-industrial) global climate variability:

Antartic Vostok ice core: D/H ratio in ice

Temp
18O/16O

ratio in carbonate sediments 800 600 400 200 0

Age (103 years before present)

Augustin et al., 2004

Isotopic records allow us to place more recent records into a larger context: Q What is natural variability? What is forced by industrial activity? Where is this headed? Inferred relative temperature (oC)

Is this normal ?

Multiple temperature proxy records from: ! tree rings, ! isotopic composition of snow, coral, stalactites ! and other sources IPCC Climate Change, 2007

Timescale of Hominid evolution: Geochronology of volcanic rocks

40K

! 40Ar

! Knowledge of decay kinetics ! Timing of volcanic eruptions ! Quantify sediment scale ! Antiquity of hominid fossils

Homo erectus: ~1.8 million years ago Koobi Fora Formation, Lake Turkana McDougall and Harrison, 1999

Radiocarbon dating Quantify the age of C-containing organic materials up to ~62,000 years: Archaeological sites nuclear reaction in atmosphere:
14N

+ n ! 14C + p

radioactive decay in dead organic matter:

14C

! 14N

West Antartica Ice Sheet Holocene Deglaciation Stone (2003) Ice surface lowering over time

E A S R s s D H

Mt. Darling, Antarctica

Glacial erratic

Text books:
Chart of the Nuclides, Lockheed Martin (Required): $25 check give to D. Shuster Check payable to UC Regents, memo = EPS 124/224 Radiogenic Isotope Geochemistry, A.P.Dickin (Required): ~$50 used paperback (Amazon) Introductory Nuclear Physics, K.S.Krane (Recommended): ~$75 used hardback (Amazon) Principles of Stable Isotope Distribution, R.E.Criss (Recommended): ~$20 used (Amazon)

Isotope Geochemistry Iso-topos (!opos) = same place

First use: Soddy (1913)

Chart of Nuclides

Protons

Neutrons

Introduction to Nuclear Physics

(an historical perspective) Henri Becquerel (1896)

! ! !

Potassium uranyl sulfate K2UO2(SO4)2 H2O Some kind of radiation from the salt blackened photographic plate (which penetrated paper, glass and other solid matter) Intensity of radiation " amount of uranium

Marie Sklodowska Curie & Pierre Curie (1898)

! ! ! ! ! ! !

Rays are generated by uranium Natural U-ore is more radio-active than pure Uranium Intensity of radiation shown to be a function of time Isolated other radioactive elements: polonium, radium, actinium First use of the word radio-active (Curie & Curie, 1898) Samples with concentrated Ra heated up (100 cal/hour/g Ra) Thorium is radioactive

Rutherford and Thomson (1899) ! ! ! ! ! Studied the nature of rays Radioactivity causes ionization in air Rutherford discovers two types of radiation (Rutherford, 1899) Terms # and $ radiation Both types of radiation absorbed by Al foil ! # rays stopped by thin foil ! $ rays only stopped with much thicker (x100) foil

Bragg (1904) ! introduces the concept of range for " particles, finding that " particles emitted from different elements have different ranges

Incident intensity

Foil absorption experiments

!o
! (d)

d
foil

!o
Intensity ! (d)

foil thickness (d)

Incident intensity

Foil absorption experiments

!o

d
foil

! (d) = !o! e-d

Where: ! = intensity through d !" = incident intensity = absorption coefficient d = foil thickness

!o
Intensity ! (d)

foil thickness (d)

Rutherford and Thomson (1899) ! ! ! ! ! Studied the nature of rays Radioactivity causes ionization in air Rutherford discovers two types of radiation (Rutherford, 1899) Terms # and $ radiation Both were absorbed by Al foil ! # rays stopped by thin foil ! $ rays only stopped with much thicker (x100) foil Rutherford postulates an exponential law for $ rays absorption
Where: ! = intensity through d !" = incident intensity = absorption coefficient d = foil thickness

I = I 0e

! d

Bragg (1904) ! introduces the concept of range for # particles, finding that # particles emitted from different elements have different ranges

Discovery of 3 types of radiation: #, $ and %& ! ! !

# and $ rays were recognized as streams of charged particles:

! using magnetic and electrostatic deflections

$ rays are negatively charged: # rays are positively charged:

! electrons moving with almost c (speed of light)

! charge/mass ratio is found to be ~1/2 that of H+, ! velocity is ~ c / 10

% rays (Villard, 1900) are not deflected in a magnetic field:

! found to be high energy electromagnetic radiation, ! more powerful than $ rays

appear after a few days

# rays emitted into an evacuated chamber caused detectable Helium gas to

! (it had already been found that U and Th ores were rich in He) ! ! # = He++

Rutherford-Soddy transformation hypothesis ! ! ! ! ! ! ! ! Noticed bursts in electrometer readings, other than radiation Could condense a high atomic weight gas (Radon)
then its radioactivity diminished rapidly (time scale)

Decreasing radiation intensity shows characteristic time scale

! depended on the radioactive substance

Radioactivity is accompanied by the transformation of atoms - uranium-x was discovered (234Th) - thorium-x was discovered (224Ra) Radiation is a by-product of transformations Transformation is at a subatomic level

Statistical nature of radioactivity (Schweidler, 1899) Disintegration probability

pdecay " !t pdecay = #!t

# = decay constant Probability of survival after $t

psurvive = 1 " #!t

And for a time t=n$t (a few $t)

psurvive (t ) = (1 " #!t ) n

As $t ' zero and

(1 " !#t ) = e " !#t (1 " !#t )n = e "!n#t = e "!t

For a large number of radioactive atoms (N(t)):

N (t 2 ) = e !" ( t2 !t1 ) N (t1 )

Also the solution to differential equation decay rate

dN = "!N dt

# of parent atoms

dN = !#dt N
N (t2 ) t2

N ( t1 )

"

d ln N = ! " #dt
t1

ln N (t 2 ) ! ln N (t1 ) = !# (t 2 ! t1 ) N (t 2 ) = e ! # (t 2 ! t1 ) N (t1 )
decay rate (!N) is called activity

Radioactive Change

Rutherford & Soddy, 1903

parent ! daughter + # (or $)&

Discovering the nucleus

Thomson discovered the electron (1897) ! ! ! ! Estimated that # e- /atom % atomic weight (false) That e- mass % 1/2000 of a H atom mass (false) Concluded that most of the mass resided in the positively charged parts Through 1911 it was believed that the electrons were embedded in a positively charged mass distributed over the volume of the atom
! plum pudding model (Thomson, 1910) ! electron repulsion balanced by attraction to positive charge

Uniform + and charge distribution with an atom

Geiger and Marsden (1909) Scattering experiment not consistent with model The testable hypothesis: If uniform (+) charge density in an atom: Predicted observations:

! No deflection of in incident particle

If concentrated charge:

! Scattering of incident (#) particle

Geiger and Marsden (1909) Scattering experiment not consistent with model

Experimental setup: # source&

#&

Rutherford scattering experiments ! If positive charge uniformly distributed in foil ! no scattering is expected. ! Conversely, if charge is non uniform ! the more scattering scattered ions detected here

# particle source #(&

)&

gold foil

!! Large scattering angles ) were too frequently observed inconsistent with the diffuse charge model !! Occasionally, ) = 180o was observed! It wasas if you fired a 15-inch shell at a piece of tissue paper and it came back and hit you. (!)

Rutherford scattering experiments ! If positive charge uniformly distributed in foil ! no scattering is expected. ! Conversely, if charge is non uniform ! the more scattering scattered ions detected here

# particle source #(&

)&

gold foil

Rutherford (1911) Positive charge is concentrated at a point (later named nucleus) Predicted scattering angles using this model and classical physics

Rutherford Scattering Formula

& # $ Nt Ze ' Z a e ! 1 $ ! n(( ) = n0 16r 2 $ 1 M v 2 ! 4&( # sin $ $ ! ) ) ! %2 " %2"

n0 = # incident " particles n(!) = # " particles scattered at angle ! t = thickness of scattering foil N = # nuclei/unit volume in foil r = distance between the scattering point and the photo plate M" = mass of alpha v" = velocity of alpha Z = atomic # of scattering material Za = 2 e = unit charge

The Rutherford model ! Was confirmed by systematic scattering experiments ! Led to the determination of nuclear charges ! Led to the realization that the atomic # of an element was equal to its nuclear charge (and # of electrons)

Rutherford Scattering Formula

Size of the nucleus ! Electrostatic repulsion predicts that the radius of the nucleus must be smaller the distance of closest approach of the " particles

# particles

nucleus distance d

when the # is at at the distance d from the nucleus, it has a potential energy of:

2 Ze 2 d
! for an # scattered at 180, the potential energy at its turn around point is equal to its original kinetic energy, T": 2 Ze 2 T! = d 2 Ze 2 d= T!

Example:

2.6Z d= # 8 "10 !15 m T$

for Z % 30; T" % 10 MeV The volume of a nucleus is about 10-12 that of an atom The density is 1012 times of an atom (roughly 1014g/cm3)

Quantifying Rutherford scattering: Size of the nucleus

e2 4!" 0

Constant e = elementary charge &0 = vacuum permittivity

! = potential energy " = kinetic energy of incident nucleus # = angular momentum

Breakdown of Rutherford scattering