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C ivil A ircraft for R egular I nvestigation of the atmosphere B ased on an I nstrument C ontainer. C A R I B I C. Luftfrachtcontainer gefüllt mit wissenschaftlichen Instrumenten, eingebaut für einzelne Messflüge 1 – 2 Messflüge pro Monat (24 – 48 Flugstunden)

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Civil Aircraft for Regular Investigation of the atmosphere Based on an Instrument Container

C A R I B I C

  • Luftfrachtcontainer gefüllt mit wissenschaftlichen Instrumenten, eingebaut für einzelne Messflüge

  • 1 – 2 Messflüge pro Monat (24 – 48 Flugstunden)

  • 11 beteiligte europäische Institute (Koordination: MPI-C, Mainz)

  • MPI für Chemie, Mainz

  • IMK, Karlsruhe

  • IFT, Leipzig

  • DLR, Oberpfaffenhofen

  • GKSS, Geesthacht

  • Universität Heidelberg

  • UEA, Norwich, UK

  • University Lund, Sweden

  • KNMI, de Bilt, The Netherlands

  • CEA/CNRS, Paris, France

  • Universität Bern, Schweiz


CARIBIC II


PTR-MS

O3

H2O

CARIBIC II Container


>4nm

18-180nm

CARIBIC II

maiden flight

13/14 Dec 2004

Frankfurt - Buenos Aires


CARIBIC II: Status & Zukunft

  • Status

  • Anfang Dezember 2004: Fluggenehmigung Airbus A340 & Container durch LBA

  • 13/14. Dezember: Erstflug nach Buenos Aires/Santiago

  • Logistik vollständig (high-loader, LKW, test equipment etc.)

  • Einlass funktioniert mechanisch & elektrisch

  • Airbus „power management“ erlaubt noch keine Aufwärmphase vor Flug

  • (kleine) Softwareprobleme bei Master PC

  • einige Instrumente noch nicht vollständig funktionsbereit

  • Zukunft

  • Zweitflug: 18/19. Februar 2005 nach Sao Paulo/Santiago (Parallelflug TROCCINOX)

  • Danach 1-2 Messflüge (25-60 h) pro Monat

  • anvisierte Flugziele: Südamerika, Südafrika, Ost Asien, Ostküste Nordamerika

  • 2005: beheben aller technischer Probleme, keine neuen Geräte

  • Veröffentlichungen & Anträge schreiben


Mess-Zelle (p,T const.)

Laser

Sample Detektor

Referenz Detektor

Reiner Absorber

Referenz-Zelle ([c] const.)

Tunable Diode Laser Absorption Spectroscopy (TDLAS)zur Messung von D/H, 17O/16O und 18O/16O in H2O

Christoph Dyroff

Lambert-Beer

σ(ν) Absorptionsquerschnitt

NMolekül Konzentration

LAbsorptionlänge

Aufeinander abgestimmt


Erste Messspektren bei 1.37μm, L~40 cm

0.10 nm


central motivation of atmospheric isotope studies is to better understand the budget of the examined trace constituents, i.e. to quantify source/sink strenghts, chemical processing, photolysis rates, transport fluxes etc.

What we can learn from isotope measurements in the atmosphere?

d - notation

e.g. d18O(H2O) = (Rsample / RV-SMOW – 1) * 1000 o/oo

with R = 18O/16O


Isotope fractionation processes

  • Phase transitions e.g. vapour pressure isotope effect

  • Chemical reactions

  • Kinetic fractionation diffusion, transport

  • Photolysis rates

  • (Radioactive decay)


isotope ratiotrace gas

hydrogenD/H (T/H)H2O, CH4, H2

carbon13C/12C (14C/12C)CO2, CH4, CO (C2H6, C3H8, …)

oxygen17O/16O,18O/16OH2O, CO2, CO, N2O, O3 (NO2, …)

nitrogen15N/14NN2O (NH3, NH4, NO2, NO3, …)

(10Be/7Be, 34S/32S)

Isotopes measured in the atmosphere

Standard Mean Ocean Water (SMOW) D/H 155.76 · 10-6

17O/16O 379.9

18O/16O 2005.2

PeeDee Belemnite (PDB)13C/12C11180

17O/16O 385.9

18O/16O 2067.2

Air (AIR)15N/14N 3676.5


solar radiation

meteorites,

asteriodes,

comets

ablation

+

evaporation

Isotope fractionation effects

CHEMICAL

REACTIONS

stratosphere

PHOTOLYSIS

Tropopause

8 – 16 km

gas-particle

transformation

condensation

+

evaporation

stratospheric

tropospheric

Exchange (STE)

free

troposphere

CHEMICAL

REACTIONS

sedimentation + rainout

boundary layer

1 – 2 km

terrestrial

radiation

volcanism

condensation

+

sublimation

biosphere

mankind

dissolution

condensation

evaporation

effusion

+

deposition

sedimentation

ices


d17O – d18O plot


O3 formation: rate coefficient ratios


CO2

O(1D)

H

H2O

O

OH

HNO3

H2O

„Transfer“ of isotope anomaly

SO42-

S(IV)aq

NMHC

O3

CO

NO

NO2

at ground

O3

N2O

NO3


MIF

dHDO = - (600-800)o/oo

dH218O = - (100-160)o/oo

DH217O = 0o/oo(= d17O – 0.52 * d18O)

ice lofting

MDF

kinetic

fractionation

vapor pressure

isotope effect

Processes controlling H2O isotopomers

30 km

T R A N S P O R T

+ C H E M I S T R Y

CH4 oxidation

H2O  HOx,, Ox

23 km

17 km

8 km

T R A N S P O R T


Isotope fractionation of H2O

a = 1 – ea fractionation factor

e fractionation

Raleigh fractionation

dRcondensate = a(T) · RgasRgas(t) = Rgas(0)·fa-1

vapour pressure istope effect (vpie)

avpie

kinetic fractionation

akin = S(T) / [avpie· D/Di ·(S(T)-1) + 1] S(T) oversaturation


H2O isotope observations at ground

Meteoric Water Line (MWL) (in precipitation)

dD(H2O) = 8.0 ·d18O(H2O) + 8.6(in per mil)


IAEA / WMO networkfor H2O isotope composition in monthly precipitation


Local MWL inwater vapour at Heidelberg 1981-2000


H2O isotope observations at ground

Meteoric Water Line (MWL) (in precipitation)

dD(H2O) = 8.0 ·d18O(H2O) + 8.6(in per mil)

Temperature effect

dD(H2O) = 8.0 ·d18O(H2O) + 8.6(in per mil)


d18O(H2O) vs. T in water vapour at Heidelberg 1981-2000


H2O isotope observations

airborne sampling at 50-80°N, DI-IRMS measurement in the laboratory

Zahn, 2001


Kuang et al., GRL, 2003

Webster et al., Science, Dec. 2003

H2O isotope observations


Simulated Isotope Profiles


Origin of O of freshly produced OH

O isotopism of OH controls dO(H2O) !

> 99 % of all H2O molecules produced in the middle

atmosphere are due to H abstraction by OH:

CH4 + OHH2O + CH3

CH2O + OHH2O + HCO

HCl + OHH2O + Cl

OH + OHH2O + O(3P)

H2 + OHH2O + H

What reactions form new OH bonds ?

X + O2HOx + Y

X + O3HOx + Y

X + O(1D)HOx + Y

O exchange:OHx + O2, NO, H2O


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