06 Water and The Hydrosphere
06 Water and The Hydrosphere
It is hard to imagine any part of the Earth system The water molecule, H2O, structurally
that is more essential than or that has as many
different functions as the water of the hydro- O
sphere. In particular, the presence of a mobile Ai05X
liquid phase, with its long list of special chemi- H H
cal and physical properties, must be clearly is a bent molecule with a very strong permanent
identified as the main feature of Earth that dipole moment. This dipole is the result of the
separates it from the other terrestrial planets or negatively charged O atom and the two posi-
from any known astronomical object. Close to tively charged H atoms (the whole molecule
home, the "terrestrial planets," Earth, Mars, and being neutral). The existence of this charge
Venus are presumed to have accreted similar separation arises due to the near orthogonality
abundances of "excess volatiles" - H2O, CO2, of the orbitals of the bonding electrons of the
etc. - but evolved very differently. Even in the central O atom, while its large magnitude arises
earliest stages of planetary evolution, liquid comes from the lack of shielding of the bonding
water provided a medium in which chemical electron and the small size of the O atom.
reactions occurred between atmospheric CO2 The permanent dipole moment is so strong
and the minerals in primitive igneous rocks to that it permits the function of what are called
allow the precipitation of carbonate minerals hydrogen bonds between the highly electronega-
and to prevent a runaway greenhouse effect. tive O atom of one molecule and a nearby
While no exact chronology or quantification of hydrogen atom of another molecule (see Fig. 6-
this early chemical event can be given, it seems 1). The hydrogen bond is not a chemical bond in
clear that some such process prevented the the ordinary sense of the forces that hold mole-
accumulation of all of the Earth's CO2 and H2O cules together, which can be deduced from its
(as a vapor) in the atmosphere at the same time. strength of ca. 20 kj/mol. Ordinary molecular
This would have caused the Earth to be moj'e or bonds have typical strengths (energy required to
less like Venus - a condition from which there break them) of a few hundred kj/mol.
would appear to be no return to our present It is the hydrogen bonds of water that give
state. Before embarking on a description of this it unique physical and chemical properties,
niost important reservoir, it is useful - perhaps characteristics that set it apart from all of the
necessary - to reflect on the special properties of other molecules formed from elements near the
water itself. We can then proceed to a discussion top of the periodic table. Table 6-1 compares
of how the hydrosphere works. several key properties of water to selected
Earth System Science Copyright 2000 Academic Press Limited
ISBN 0-12-379370-X All rights of reproduction in any form reserved
110 Patricia C. Henshaw, Robert J. Charlson, and Stephen J. Barges
compounds and polar organic species. Com- disciplines. The Earth and its atmosphere, in the
pounds that will not significantly dissolve in broadest view, are a complex, intimately
water (i.e. saturated solutions with concentra- coupled system of chemical, physical, and bio-
tions less than ca. 10 ~^ M) include aliphatic and logical cycles, and water, with its myriad unique
aromatic hydrocarbons, as well as plastics and chemical and physical properties, plays a part in
many other polymers. almost all of them.
To understand the role water plays in global
cycles, it is necessary to first understand the
6.1,2 The Right Abundance of Water to mechanics of the water cycle. The hydrologic
Support Life cycle is driven by solar radiation, which pro-
vides the energy necessary to overcome latent
As can be seen in Fig. 2-1 (abundance of ele- heat capacities involved in phase changes. Grav-
ments), hydrogen and oxygen (along with ity plays a key role in returning condensed
carbon, magnesium, silicon, sulfur, and iron) water to the surface as precipitation, and via
are particularly abundant in the solar system, runoff from the continents to the oceans. At the
probably because the common isotopic forms of simplest level, the global water cycle results
the latter six elements have nuclear masses that from imbalances between precipitation and eva-
are multiples of the helium (He) nucleus. potranspiration (ET) at the ocean and land
Oxygen is present in the Earth's crust in an surfaces. Globally, the oceans lose more water
abundance that exceeds the amount required to by evaporation than they gain by precipitation,
form oxides of silicon, sulfur, and iron in the whereas the land surface receives more precipi-
crust; the excess oxygen occurs mostly as the tation than is lost through ET; runoff from the
volatiles CO2 and H2O. The CO2 now resides land surfaces then balances the ocean-atmos-
primarily in carbonate rocks whereas the H2O is phere water deficit. The hydrologic cycle is
almost all in the oceans. significantly more complex than this simple
While it is clear that the hydrosphere is a description would suggest. In addition to the
significant portion of the planet's mass, there is atmosphere, oceans, and rivers, significant
not, at least currently, so much water that the amounts of water are stored in groundwater,
continents are submerged. Conversely, the glaciers and ice sheets, soil moisture, and, to a
oceans are large enough that their surface area smaller extent, biomass. Figure 6-3 shows a
would never become an important limiting schematic of the global hydrologic cycle, with
factor in the hydrologic cycle. Although there storages in km^ and fluxes in km^/yr.
have been many shifts in the balance of the
hydrosphere, this condition has prevailed since
the biosphere began to evolve. The presence of Atmosphere 12.9x103 (8 days)
Calculation of the global water balance is a extensive knowledge of hydrologic and meteor-
nontrivial problem. Gross storage volumes are ologic parameters. Consequently, numerous
calculated predominantly by multiplying sur- estimates of storage and flux volumes exist for
face areas by estimated average depths the hydrologic cycle; the representation in Fig. 6-
(UNESCO, 1978). While modem remote sensing 3 was selected for its completeness. Some of the
technology has made it possible to determine variability in estimates of the global water bal-
areal extents of surface reservoirs, such as ance is reflected in the reservoir storage values
oceans, lakes, and ice sheets quite accurately, shown in Table 6-2.
estimations of depths or thicknesses are still
highly uncertain and often subjective. For exam-
ple, the wide variations in groundwater esti- 6.2.7 Reservoirs
mates can often be attributed to differing
interpretations of the extent of groundwater Figure 6-3 shows the hydrologic cycle as seven
into the Earth's crust. Similarly, soil moisture primary reservoirs interconnected by a number
depths vary from less than a meter to tens of of water fluxes. The role of each reservoir in the
meters or more, so global soil moisture averages hydrologic cycle and its connections with other
are by necessity highly subjective. Even more cycles is briefly summarized below, in order of
well-defined reservoirs, such as oceans or lakes, storage volume.
cannot be accurately quantified without com-
plete knowledge of their bathymetry and verti- 6.2.7.7 Oceans
cal temperature profiles, an impossible
requirement on a global scale. The oceans are by far the largest reservoir in the
Although fluxes of precipitation and river hydrologic cycle, containing more than 25 times
discharge can be quite accurately determined as much water as the rest of the reservoirs
on a local scale, large portions of the globe, combined. As another means of comparison,
especially the oceans and Antarctica, are essen- the volume of water in the oceans is four orders
tially ungauged, requiring extensive extrapola- of magnitude larger than that in the next most
tion of existing data. Evaporation fluxes are visible reservoir, the world's lakes and rivers.
even less well known, since calculation requires The oceans are also one of the Earth's primary
114 Patricia C. Henshaw, Robert J. Charlson, and Stephen J. Barges
heat reservoirs and have absorbed approxi- water from the last ice age, which is essentially a
mately half of the CO2 emitted to the atmos- nonrenewable supply.
phere; consequently the oceans play an Groundwater is fed through infiltration and
important role in climate. Coupled with atmos- percolation through the soil and is recycled via
pheric circulation, surface and thermohaline transpiration through plants, interflow into
circulations in the oceans transfer heat from river networks, and some direct discharge to
low to high latitudes and provide a modulating the ocean. This reservoir is extremely important
effect on global temperatures. in global water resources, though reserves in
some areas are threatened by overdraft and
pollution.
6.2.7.2 Glaciers and ice sheets
cycling, mainly via transpiration through land how long it takes to replace the entire storage in
plants and, to a lesser extent, via photosynthesis. a reservoir. In a steady-state system, which is a
Soil-plant interactions are also the key determi- reasonable approximation for Earth cycles on
nants of land surface evaporation; in vegetated geologic time scales, turnover times also provide
continental areas, most evaporation of soil a sense of how long it will take a reservoir to
moisture occurs by virtue of transpiration. In respond to perturbations in the cycle. Reservoirs
addition to evaporation, the land surface con- with short turnover times are most sensitive,
tributes to albedo, though surface effects have while those with longer turnover times respond
proven difficult to parameterize in global cli- more slowly and can often act as buffers on
mate models. Albedo is a strong function of the shorter time scales.
availability of liquid water. Arid areas (deserts) The enormous volume of the oceans results in
have very high albedo compared to vegetated an average turnover time of more than 2600
land. Consult Chapter 17 for more information years, compared to less than 10 days for atmos-
on climate considerations. pheric water. Although the reservoir is much
smaller than the oceans, the cryosphere has the
6.2.7.6 Atmosphere longest turnover time due to the small input
flux. Average turnover times for all seven reser-
Although it is one of the smallest reservoirs in voirs, calculated from the data in Fig. 6-3, are
terms of water storage, the atmosphere is prob- shown in Table 6-3.
ably the second most important reservoir in the Many hydrologic reservoirs can be further
hydrosphere (after the oceans). The atmosphere subdivided into smaller reservoirs, each with a
has direct connections with all other reservoirs characteristic turnover time. For example, water
and the largest overall volume of fluxes. Water resides in the Pacific Ocean longer than in the
is present in the atmosphere in solid, liquid, and Atlantic, and the oceans' surface waters cycle
vapor forms, all of which are important compo- much more quickly than the deep ocean. Simi-
nents of the Earth's natural greenhouse effect. larly, groundwater near the surface is much
Cycling of water within the atmosphere, both more active than deep reservoirs, which may
physically (e.g. cloud formation) and chemi- cycle over thousands or millions of years, and
cally, is also integral to other biogeochemical water frozen in the soil as permafrost. Typical
cycles and climate. Consult Chapter 17 for more range in turnover times for hydrospheric reser-
details. voirs on a hillslope scale (10-10^ m) are shown
in Table 6-4 (estimates from Falkenmark and
Chapman, 1989). Depths are estimated as typi-
6,2,2 Turnover Times cal volume averaged over the watershed area.
Global freshwater reserves (discounting pol-
Average turnover time (defined as storage lution) are a small percentage of global water,
volume divided by annual inflow or outflow accounting for only 35 x 10^ km of the total
volume, assuming steady state) is a measure of 1.386 X 10^ km^ global water supply (UNESCO,
Table 6-4 Hillslope scale turnover times since freshwater volume is essentially equal to
non-marine storage and net evaporation is the
Reservoir Depth (mm) Turnover times only output flux from the oceans, this may be
Atmosphere 25^ 8-10 days taken as a reasonable estimation. For practical
Plants 5-50 Hours-days purposes, freshwater resources available to
Streams/rivers 3 Weeks humans cycle more rapidly, but since 97% of
Lakes / reservoirs Months-years freshwater is stored in ice, the global average
Soil moisture 10-10^ Years turnover is much longer.
Groundwater loMo^ Days-10^ years^
^ Global average.
^ Longer turnovers associated with large watershed 6.2J Fluxes
areas.
Robert Horton, an influential pioneer in the field
of hydrology, developed one of the first com-
1978). Assuming an input flux equal to oceanic prehensive representations of the hydrologic
evaporation, this w^ould give a turnover time of cycle in 1931. His original diagram. Fig. 6-4,
about 750 years. The turnover time analysis is illustrates the processes by which water moves
not strictly correct since freshwater resides in a between the Earth's hydrologic reservoirs.
number of interconnected reservoirs; however. Hydrologic fluxes can be summed up in four
Fig. 6-4 The fluxes of the hydrologic cycle, developed by Robert Horton (1931).
Water and the Hydrosphere 117
6.2.3.3 Runoff
PRECIPITATION IN INCHES
Red River
N. Saskatchewan
S. Saskatchewan
St. Lawrence
Susquehanna
Niagara
Assiniboine
Colorado
Mississippi
Missouri
Ohio
Columbia
Snake
Vuoksi
V. Gota
Rhine
Loire
Seine
Garonne
Rhone
Po
Ebro
Guadalquivir
Elbe
flUS^.B
Vistula
Oder Central
Danube Europe
Dvina
Don
Volga Western
Neman
Ural U.S.S.R
Kolyma
Amur
Ob
Yenisei Eastern
Lena U.S.S.R
Nile
Senegal
Niger
Chari
Congo Africa
Orange Dry period
Limpopo
Humid period
Amazon
Parana
Sao Francisco South
Ametica
Godavari
Mekonc South eastern
Asia
1800 1850 1900 1950 2{XX)
Fig. 6-10 Long-term global streamflow trends. Wet and dry periods from the historical record of 50 major
rivers. (From Probst and Tardy, 1987.)
The precipitation record shows a mild Runoff sensitivity, particularly in arid and
decrease in rainfall for May, June, and July over semi-arid climates, is largely a result of sensi-
the last 20 years of record. However, runoff tivity in soil moisture response. If rainfall
decreased to less than half the historical average amount and frequency decrease, more soil
for May and June over the same period, and moisture is lost to evapotranspiration, creating
reduced runoff persisted into December, despite a soil moisture deficit that must be replaced
a return to normal or above normal precipitation before surface runoff or significant ground-
levels over the latter half of the year. water flow returns. The converse also tends to
124 Patricia C Henshaw, Robert J. Charlson, and Stephen J. Burges
Monthly Average
m (1911 - 1994)
In addition to biogeochemical cycles (discussed
S (1950 - 1994) in Section 6.5), the hydrosphere is a major
(1975 - 1994) component of many physical cycles, with cli-
mate among the most prominent. Water affects
the solar radiation budget through albedo (pri-
marily clouds and ice/snow), the terrestrial
radiation budget as a strong absorber of terres-
trial emissions, and global temperature distribu-
tion as the primary transporter of heat in the
ocean and atmosphere.
Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec
Month 6.4,1 Water and the Energy Balance
through the Bowen ratio, which is the ratio of particularly at the regional scale important for
sensible heat to latent heat flux at the surface. water resources, are much more speculative
The Bowen ratio, R, can be estimated from (IPCC, 1996a).
atmospheric properties as follows:
SH T,
R 0.66- (4) 6.4.2.7 Climate feedbacks
LE eo 1000
where SH = sensible heat (Energy/unit time and In its assessment of climate change, the IPCC
unit area); LE = latent energy flux (Energy/unit (1990) identified five hydrosphere-related feed-
time and unit area); TQ = surface temperature back mechanisms in the climate system likely to
(C); Ta = reference level air temperature (C); eo be activated by increased greenhouse gas con-
= saturation vapor pressure (mbar); e^^ = atmos- centrations in the atmosphere. These feedbacks
pheric vapor pressure (mbar); p = atmospheric are briefly described below; for more detailed
pressure (mbar). discussion of the climate system, refer to Chap-
For saturated surfaces, the Bowen ratio can ter 17.
then be used to calculate evapotranspiration as a
residual of the surface energy balance (Penman, 6.4.2.1.1 Atmospheric moisture. Short resi-
1948). Since direct measurement of ET is difficult dence times and rapid phase changes for water
and expensive, the energy balance method is in the atmosphere give it a disproportionately
fairly common. large influence on climate. Changes in atmos-
pheric moisture affect cloud properties and are
related to the cloud feedback mechanisms dis-
6.4.2 Climate Feedbacks and Response to cussed below. In addition, water vapor is the
Global Warming most effective greenhouse gas due to its large
heat capacity and absorption spectrum; thus
Five components of the hydrosphere play major expected increases in atmospheric vapor content
roles in climate feedbacks - atmospheric mois- (due to accelerated evaporation) would have a
ture, clouds, snow and ice, land surface, and positive feedback effect. Increased evaporation
oceans. Changes to the hydrologic cycle, among and associated release of latent heat to the atmos-
other things, as a result of altered climate condi- phere (upon condensation) would warm the
tions are then referred to as responses. Inter- troposphere, increasing its moisture storage
actions with climate can best be explored by capacity. Additional water vapor then traps
examining potential response to a climate more terrestrial radiation, enhancing the green-
perturbation, in this case, predicted global house effect and further warming the tropo-
warming. sphere. Although runaway warming would be
Current debate regarding the role of the prevented by changes in lapse rates to increase
hydrologic cycle in climate focuses on potential the flux of water vapor from the troposphere to
responses to anthropogenically induced global higher altitudes, the predicted net effect of the
warming through an enhanced greenhouse atmospheric moisture feedback is surface and
effect due to increased atmospheric CO2 and atmospheric warming (Ramanathan, 1988).
other gases. Based on GCM simulation results,
the Intergovernmental Panel on Climate Change 6.4.2.1.2 Clouds. Cloud feedback mechanisms
(IPCC) has concluded that global mean surface are among the most complex in the climate
atmospheric temperature will increase by 1.0 to system, due to the many disparate roles played
3.5C in the next century, though this will be by clouds, which control a large portion of the
distributed unevenly over the Earth, with the planetary albedo but also trap terrestrial radia-
most significant warming expected at high lati- tion, reducing the energy escaping to space. To
tudes. Warmer temperatures are expected to complicate matters further, different types of
accelerate the hydrologic cycle, though the mag- clouds behave differently in the same environ-
nitude and distribution of hydrologic changes. ment. In the present climate mode, clouds have
726 Patricia C. Henshaw, Robert J. Charlson, and Stephen J. Barges
a global mean cooling effect, but the sign of resistance in plants, with the potential to reduce
cloud feedback in climate models remains con- transpiration loss per unit leaf area by up to
troversial. 50%, but also increases plant growth. The net
Considerable uncertainty about the types of effect on transpiration is uncertain (Rosenberg et
clouds that will increase due to greenhouse al, 1990).
warming is the primary obstacle to predicting
cloud feedback. Higher cloud top heights, 6.4.2.7.5 Ocean circulation. Paleoclimate evi-
assuming no change in cloud cover or water dence has linked changes in thermohaline circu-
content, might result in surface warming due to lation and the formation of North Atlantic Deep
greater capacity to absorb outgoing (terrestrial) Water (NADW) with several of the major cli-
radiation. Conversely, higher water content mate shifts of the last glacial period. Therefore,
would increase cloud albedo and result in net ocean circulation feedback will probably play
surface cooling potentially capable of balancing some role in determining the hydrologic and
additional greenhouse warming (Chahine, climatic response to greenhouse warming,
1992). Ocean surface warming has also shown a though long ocean response times could make
moderating effect, increasing convective activity this a less important feedback in the short term.
and the formation of high-albedo cirrus clouds The mechanism for thermohaline response is the
(Chahine, 1992). influx of low-density freshwater into the polar
oceans due to precipitation and the melting of
6.4.2.7.3 Snow-ice albedo. Although cryo- glaciers and icecaps. Since density is the domi-
spheric processes remain among the greatest nant driving force for sinking, increased high-
sources of uncertainty in climate modeling, latitude precipitation and/or significant melting
models have consistently shown enhanced events could trigger a slowing or stoppage of
warming at the poles, resulting in melting of deep-water formation. As a result, global circu-
sea ice and less snow and ice cover. Since snow lation and poleward heat transfer would be
and ice have higher albedos than the underlying greatly reduced, lowering surface temperatures
land surfaces and oceans, this results in and providing a negative feedback on global
increased absorbed atmospheric radiation at warming. Broecker (1997) hypothesized that a
the surface and further warming. Increased net increase in freshwater input to the North
vegetative cover from the predicted poleward Atlantic of 50% - which is within predicted
migration of currently more temperate biomes ranges - would disrupt the salt balance suffi-
would also reduce surface albedo of the polar ciently to trigger an instability in and reorgani-
regions (IPCC, 1998). Significant melting of sea zation of the thermohaline circulation.
ice could also result in changes to ocean thermo-
haline circulation, as has been observed at sev-
6.4.2.2 Hydrologic response
eral points in the paleoclimate record (see
below).
Accelerated hydrologic processes are predicted
6.4.2.7.4 Land surface/biosphere. The com- to result in an increase of global mean precipita-
plexity and high regional variability of land tion by 3 to 15%, though changes in regional
surface and biosphere effects make them ex- precipitation would likely vary by 20%
tremely difficult to model, though some general (Schneider et ah, 1990). Like temperature, pre-
feedbacks have been identified. Changes in pre- cipitation changes would be unevenly distribu-
cipitation (amount and temperature) and evap- ted, with high- and most mid-latitude areas
oration regimes will affect soil moisture storage receiving higher precipitation, while rainfall in
and infiltration rates (which in turn influence the tropics may decrease. Changes in the
runoff magnitude). Higher evaporation rates amount and type of precipitation (rain versus
would be expected to reduce soil moisture and snow) also have important implications for
runoff, though this could be partially offset by runoff magnitude and timing, with regional
reduced transpiration caused by elevated CO2. changes in runoff predicted to vary by as much
Increased carbon dioxide increases stomatal as 5 0 % (Schneider et ah, 1990). Current
Water and the Hydrosphere 127
phosphorus is transported in both dissolved and environments (high precipitation and runoff)
particulate form. tend to have low concentrations of sodium-
Phosphorus is extremely important in bio- chloride-dominated salts. Evaporation-domi-
logical reactions and is thus cycled through nated rivers (low precipitation and runoff) are
biological systems many times before it ulti- also NaCl dominated but with high total salt
mately reaches the ocean. Phosphorus cycling is concentrations. Areas with moderate precipita-
particularly important in lake and wetland sys- tion and runoff generate rock-dominated river
tems, where it is often temporarily stored in chemistry, with moderate concentrations of cal-
sediments. Consequently, the groundwater link cium bicarbonate salts (Gibbs, 1970). Natural
is more important in the phosphorus cycle than salt concentrations can be altered or over-
in other elemental cycles. Concentrations of whelmed by human activities, particularly by
dissolved P in groundwater depend on bio- irrigated agriculture.
logical and inorganic reactions.
iMIiJI ll
S 150
I
Co
100 with the direct physical changes discussed
? 50 above.
^ 0 These and other direct human impacts on the
O N D J F M A M J J A S
hydrosphere are unlikely to affect the global
Fig. 6-12 Comparison of mean monthly averaged hydrologic cycle, particularly since humans
daily discharges for the Columbia River at The Dalles, have not had a great deal of success in manip-
Oregon for water years 1915-1924 (1 Oct. 1914-30 ulating the water balances of the ocean and
Sep. 1924) and 1985-1994. (Data from US Geological atmosphere, the largest and most sensitive reser-
Survey, Station 14105700.) voirs in the system, respectively. Significant
anthropogenic effects on the hydrologic cycle
are much more likely to arise from indirect
May-June runoff peaks, 2 to 2.5 times the annual changes, most notably human-induced climate
average runoff in the 1915-1924 period prior to change.
dam construction, v\^ere barely 1.5 times the
average flow between 1985 and 1994. Mean-
while, autumn low flows during the 1985-1994 6.8 Conclusion
period are close to the mean annual flow, com-
pared to low flows at about half the mean prior Cycling of water between the atmosphere, land
to river regulation. surface, and oceans is important not only to
The consequences of this regulated system humans and other organisms, which rely on
include significantly lower total discharge water to live, but in maintaining balances in
(beyond what would be expected from climate other cycles as well. Hydrologic fluxes, predo-
variability), ecological effects of altered fresh- minantly rain and rivers, transport significant
water inputs to the Pacific, and altered sediment amounts of carbon, nitrogen, sulfur, and phos-
budgets due to sediment trapping behind dams. phorus, among other elements, between reser-
One unintended result of the changed hydro- voirs in their own biogeochemical cycles. Rivers
graph has been reduced autumn and winter are also a major link in the tectonic cycle,
surface salinity from the mouth of the Columbia transporting sediment eroded from upland
along the North American coast to the Aleutian areas to inland basins and to the oceans. The
Island chain, which has potentially negative heat capacities and physical properties of all
ecological consequences for endangered salmon phases of water also give the hydrosphere an
runs. important role in the global heat balance and
Regional water balances are also altered by climate.
agricultural and domestic water uses drawing To this point, direct human impacts on the
on underground aquifers, increasingly at rates hydrosphere have remained restricted to the
that exceed natural recharge capability and regional scale. Although they can still be impor-
result in groundwater overdraft. Pollution of tant, particularly in terms of water supply, these
surface and groundwaters, though it has no direct manipulations of the hydrologic cycle are
physical effect on the water cycle itself, results unlikely to affect the global water balance sig-
in a loss of freshwater resources in addition to nificantly. However, this is not to suggest that
the effects on balances in other biogeochemical the global water cycle is immune to human
cycles. influence; its close ties to other physical and
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biogeochemical cycles subject the hydrologic Dunne, T. and Leopold, L. B. (1978). "Water in
cycle to indirect effects of h u m a n impacts on Environmental Planning." W.H. Freeman, San
these cycles as well. The m o s t i m m e d i a t e h u m a n Francisco.
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the sulfur cycle, carbon cycle, a n d biosphere, as water chemistry. Science 170,1088-1090.
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