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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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C a r i b i c

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

CARIBIC II


Caribic ii container

PTR-MS

O3

H2O

CARIBIC II Container


C a r i b i c

>4nm

18-180nm

CARIBIC II

maiden flight

13/14 Dec 2004

Frankfurt - Buenos Aires


Caribic ii status zukunft

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


C a r i b i c

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 37 m l 40 cm

Erste Messspektren bei 1.37μm, L~40 cm

0.10 nm


What we can learn from isotope measurements in the atmosphere

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

Isotope fractionation processes

  • Phase transitions e.g. vapour pressure isotope effect

  • Chemical reactions

  • Kinetic fractionation diffusion, transport

  • Photolysis rates

  • (Radioactive decay)


Isotopes measured in the atmosphere

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


Isotope fractionation effects

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


D 17 o d 18 o plot

d17O – d18O plot


O 3 formation rate coefficient ratios

O3 formation: rate coefficient ratios


Transfer of isotope anomaly

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


Processes controlling h 2 o isotopomers

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 h 2 o

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


H 2 o isotope observations at ground

H2O isotope observations at ground

Meteoric Water Line (MWL) (in precipitation)

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


Iaea wmo network for h 2 o isotope composition in monthly precipitation

IAEA / WMO networkfor H2O isotope composition in monthly precipitation


Local mwl in water vapour at heidelberg 1981 2000

Local MWL inwater vapour at Heidelberg 1981-2000


H 2 o isotope observations at ground1

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)


D 18 o h 2 o vs t in water vapour at heidelberg 1981 2000

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


H 2 o isotope observations

H2O isotope observations

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

Zahn, 2001


H 2 o isotope observations1

Kuang et al., GRL, 2003

Webster et al., Science, Dec. 2003

H2O isotope observations


Simulated isotope profiles

Simulated Isotope Profiles


O isotopism of oh controls do h 2 o

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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