On the UK-scale, sulphur dioxide (SO2) dry deposition has declined at a fas
ter rate than SO2 emissions, but S wet deposition has declined at a slower
rate than emissions. Three hypotheses have been put forward to explain this
non-linear response to changes in emissions: changes in the effective rele
ase height of emissions; oxidation of SO2 may have been oxidant limited in
previous years; the canopy resistance Of SO2 has changed in response to cha
nging ammonia concentrations. Of these three hypotheses, the first has been
tested here using a 10-layer Lagrangian acid deposition model. The model r
eproduced the rate of decline of observed total S deposition but not the ma
gnitude. The mismatch in magnitude between modelled and observed UK S depos
ition is consistent with the model framework and its limitations. More impo
rtantly, the model did not reproduce the changes in the proportions of wet
and dry deposition to the UK that have been observed using two different se
ts of UK emission data. The UK-derived emissions data show a small increase
in the proportion of lowlevel SO2 sources to the total and a small decreas
e in proportion of the high-level SO2 sources over the period 1989-1994. Th
ese changes are not apparently consistent with observed changes in SO2 conc
entrations nor changes in wet and dry S deposition. Thus, it is unsurprisin
g that the modelling does not simulate the observed changes in fractions of
wet and dry deposition. The current constraints of the modelling and the e
missions data have the consequence that future scenarios of rates of change
of total S deposition may be optimistic for locations that are dominated b
y wet deposition, remote from sources. Crown Copyright (C) 2001 Published b
y Elsevier Science Ltd. All rights reserved.