Atmos. Chem. Phys., 9, 7481–7490, 2009 www.atmos-chem-phys.net/9/7481/2009/ © Author(s) 2009. This work is distributed under the Creative Commons Attribution 3.0 License. Atmospheric Chemistry and Physics Analytical treatment of ice sublimation and test of sublimation parameterisations in two–moment ice microphysics models K. Gierens and S. Bretl Deutsches Zentrum für Luft- und Raumfahrt, Institut für Physik der Atmosphäre, Oberpfaffenhofen, Germany Received: 18 February 2009 – Published in Atmos. Chem. Phys. Discuss.: 30 April 2009 Revised: 11 September 2009 – Accepted: 21 September 2009 – Published: 7 October 2009 Abstract. We derive an analytic solution to the spectral growth/sublimation equation for ice crystals and apply it to idealised cases. The results are used to test parameterisations of the ice sublimation process in two–moment bulk microphysics models. Although it turns out that the relation between number loss fraction and mass loss fraction is not a function since it is not unique, it seems that a functional parameterisation is the best that one can do in a bulk model. Testing a more realistic case with humidity oscillations shows that artificial crystal loss can occur in simulations of mature cirrus clouds with relative humidity fluctuating about ice saturation. 1 Introduction Cloud microphysical models can essentially be grouped into bulk and bin models. Bulk models describe a cloud in terms of gross quantities like total water or ice mass and total number concentration of hydrometeors. Although an assumption of the underlying size or mass spectrum of the hydrometeors is usually made, its evolution is not completely described since only the low-order moments are predicted in the model equations. Bin models instead describe a cloud in much more detail by explicitly accounting for the size or mass spectrum. Here the mass spectrum is divided into a large number of bins and the microphysical processes directly change the number of particles in the various bins (some recent examples can be found in Lin et al., 2002; Monier et al., 2006; Leroy et al., 2007, 2009). While bulk microphysics models are designed rather for computational speed than for an exact description of the evolution of a cloud’s mass spectrum, it is vice versa for the bin models which pay for more exact results with Correspondence to: K. Gierens ([email protected]) higher computational costs, that is, longer computing time and higher memory requirements. For many applications (for instance in an operational weather forecast model) it is too expensive to use a bin model, hence bulk models are needed. Nonetheless, their behaviour should be tested under a large variety of situations such that their strenghts and weaknesses become understood as much as possible. Cloud microphysical models that use a two–moment bulk scheme predict both the temporal and spatial variations of the total number and total mass of the droplets and ice crystals. The temporal change of number and mass concentrations are determined by process rates which are sometimes difficult to formulate. One example is deposition. When ice crystals grow by vapour deposition, the ice mass grows accordingly while the number of crystals is constant. This is the easy case. The difficult case arises in subsaturated conditions. When ice crystals sublimate, the ice mass decreases accordingly, while the decrease rate of crystal number cannot be formulated in a straightforward way. The prognostic equations for ice number and mass concentration (for recent examples cf. Morrison and Grabowski, 2008; Spichtinger and Gierens, 2009) contain deposition terms, DEP (for mass concentration) and N DEP (for number concentration) in the nomenclature of Spichtinger and Gierens (2009). The problem is now, that there is an equation for DEP , but not for N DEP . Harrington et al. (1995) have performed a large series of simulations to find an appropriate parameterisation for N DEP . Spichtinger and Gierens (2009) roughly followed their results and used the following simple approximation to calculate N DEP : fn = fmα , (1) where fm is the mass fraction sublimated in the current time step, fn is the desired number fraction, and α is a constant parameter. Harrington et al. (1995) suggest a range of 1≤α≤1.5 for this parameter, which is set to α = 1.1 by Published by Copernicus Publications on behalf of the European Geosciences Union. 7482 K. Gierens and S. Bretl: Analytical treatment of sublimation Spichtinger and Gierens (2009). Morrison and Grabowski (2008) use α = 1, i.e. fn = fm . The constancy of α is certainly an oversimplification, since this would mean that ice crystals in fall streaks sublimate in a similar way than ice crystals deep inside a cloud where small humidity fluctuations around ice saturation might lead to crystal loss. Hence, we deemed it worth to investigate this process in more detail and to test potential alternative parameterisations. For this purpose we will use an analytic solution to the problem, proceeding from the spectral form of the growth/sublimation equation, to be derived next in Sect. 2. From the analytical solution we compute number and mass loss fractions (Sect. 3) and derive timescales (Sect. 4). Alternative parameterisations will be tested in Sect. 5. A discussion and conclusions are presented in the final Sects. 6 and 7. but expressions like mb are always meant as (m/U M)b . With the chosen units, a certain value of a (which is a number) means that the sublimation rate of a 1 ng ice crystal is a ng/s. In this paper we use crystal masses and values of a that are typical in cirrus clouds under subsaturated conditions, i.e. the temperature is below −38◦ C, the pressure below 300 hPa and the relative humidity with respect to ice ranges from say 10 to 98%. We used b = 0.37 and a width of the mass distribution of σm = 2.85. Note that the exact values are not important for the principle considerations that follow. We introduce the following coordinate transformation: 2 Time dependent crystal mass distribution As ice crystals in a cloud generally have a large variety of sizes, bulk microphysics models take account of this variety by implicitly or explicitly assuming an underlying crystal size distribution, which can be expressed as a crystal mass distribution or mass spectrum, f (m). Crystal growth by vapour deposition or crystal sublimation changes the mass spectrum, so that it becomes also a function of time, i.e. f (m, t). The temporal change of the mass spectrum due to deposition/sublimation can be described by an equation that has the form of a continuity equation in mass space (see, e.g., Wacker and Herbert, 1983): ∂ ∂ f (m, t) = − (ṁf ). ∂t ∂m (2) f (m, t) dm can equivalently be interpreted as the time dependent probability that an ice crystal selected randomly in a cloud has a mass between m and m + dm. The probabilistic interpretation will turn out useful for the analytical derivations presented in the following. (f (m, t) has to be distinguished carefully from fractions fk which are marked by a lower index.) ṁ ( = dm/dt) is the depositional mass growth/sublimation rate of a single crystal of mass m. Koenig (1971) has shown that ṁ can be parameterized as a function of m in the simple form: m b ṁ =a . (3) U M/U T UM Here, a and b depend on temperature and pressure, and a depends additionally on the degree of ice supersaturation. For subsaturated cases, a<0. Spichtinger and Gierens (2009, their Fig. 5) show that this approximation is very good over four orders of magnitude in m. U M and U T are unit mass and unit time, for which we use 1 ng and 1 s, respectively. In the following equations we drop the reference to the units, Atmos. Chem. Phys., 9, 7481–7490, 2009 x= m1−b 1−b (4) (= const). ẋ = a That is, in the new coordinates the growth/sublimation rate is a simple constant. Let g(x) be the probability density function of x. Then the spectral growth equation obtains the simple form: ∂ ∂g g(x, t) = −a , ∂t ∂x (5) which is solved by a characteristic: (6) g(x, t) = g̃(x − at). g̃ can be any function in principle, but here we use probability density functions, of course. It is obvious that the time development of g(x, t) is merely a shift of the function as a whole along the x-axis. All central moments of order higher than one are invariant, that is, the shape of g(x, t) does not change over time. We start (t = 0) from a certain initial mass distribution (e.g., log-normal), normalized to one for the present paper: f (m, 0) dm = √ m 2 1 [ln( m0 )] exp − 2 (ln σm )2 ( 1 2π ln σm ) 1 dm, (7) m substitute m with x (this yields another log-normal with 1−b x0 = m1−b 0 /(1 − b) and ln σx = ln σm ): x 2 1 [ln( x0 )] g(x, 0) dx = √ exp − 2 (ln σx )2 2π ln σx ( 1 ) 1 dx, x (8) and then replace x with x −at, which represents the temporal evolution of the mass distribution in the x-coordinates: (9) g(x, t) dx = √ 1 2π ln σx 2 [ln( x−at x )] 1 exp − 12 (ln σ0 )2 x−at dx. x Finally, we have to substitute back x with m1−b /(1 − b), to get the desired result: www.atmos-chem-phys.net/9/7481/2009/ K. Gierens S. Bretl: Analytical treatment ofsublimation sublimation K. Gierens Gierens andand Bretl: Analytical treatment of and S.S.Bretl: Analytical treatment of sublimation 3 1 1 1.4 1.4 3 7483 1.2 1.2 0.8 0.8 1 f(m,t) 0.8 0.8 0.6 0.6 φn 0.6 0.6 φn f(m,t) 1 0.4 0.4 0.4 0.4 0.2 0.2 0 0 0.001 0.001 0.01 0.01 0.1 0.1 Crystal massmass (ng) (ng) Crystal 1 10 1 Fig.Fig. 1.1. f1.(m, t) for various times t under withwith a =with (m, t) for various times t under sublimation a = Fig. ff(m, t) for various times t sublimation under sublimation ◦ (approximatly for for −50−50 C, ◦◦250 hPa,hPa, RHRH == 98%). iRH (approximatly −50 C, 250 250 hPa, = 98%). i 98%). a−0.004 = −0.004 −0.004 (approximatly for C, t=0 i t =t = 0 (solid red,red, the the initial log–normal distribution), and t = t = 0 the (solid initial log–normal distribution), (solid red, initial log–normal distribution), and t = 10,and 30, 60, 10, 30, 30, 60, 120120 s (solid green and and blue, dashed red and (solid green dashed red blue). and blue). 12010, s (solid60, green sand blue, dashed blue, red and blue). Singularities of this formulation can can appear at negative m m Singularities of this formulation appear at negative which are are irrelevant. TheThe singularity developing at mat=m0= 0 which irrelevant. singularity developing is integrable. TheThe temporal evolution of the initially log–log– is integrable. temporal evolution of the initially Fig. normal distribution is shown in Fig. 1 for sublimation con1 afor 2connormal distribution is shown in a sublimation 1−b −(1−b)at m dition (a < 0). It is evident that in the mass coordinates the dition (a < 0). It is evident that in the lnmass coordinates the 1−b m 1 1 distribution does not retain its initial shape; deviations from 0 distribution its initial from − shape; deviations exp f (m, t) dm = does √ not retain 2 (ln σ )in2 the the initial shape are2π very 2When (1When −web)consider lnvery σpronounced. initial shape are we consider m m pronounced. initial in stead a growth situation (a > shape is much stead a growth situation (a 0) >the 0) the initial shape is much better conserved (not(not shown). A more general solution of the better conserved shown). A more general solution of the 1 equation spectral growth is presented in Appendix A. × spectral growth equation dm (10) is presented in Appendix A. b m − (1 − b)atm 3 3Mass lossloss andand number lossloss fractions Mass number fractions Singularities of this formulation can appear at negative m WeWe assume thatthat ice ice crystals havehave a minimum massmass of which are irrelevant. The singularity developing at m mofthr =m0thr is assume crystals a minimum −3 (e.g. 10 ng). Then we define for k ∈ {0, 1} the following −3 integrable. The temporal evolution of the initially log-normal (e.g. 10 ng). Then we define for k ∈ {0, 1} the following integrals which give theintotal number mass fractions of distribution is shown for and a sublimation condition integrals which give theFig. total1 number and mass fractions of the ice mass distribution exceeding the threshold: (a<0). is evident that inexceeding the massthe coordinates the iceIt mass distribution threshold: the distriZ∞ not bution does retain its initial shape; deviations from the Z∞k initial shape are pronounced. When we consider(11) instead Ik (t) := m very f (m, t)dm. Ik (t) := mk f (m, t)dm. (11) a growth situation (a>0) the initial shape is much better conmthr mthr served (not shown). A more general solution of the spectral Since f depends on time, so does Ik . Harrington et al. (1995) growth is on presented Appendix A. Sinceequation f depends time, soin does I . Harrington et al. (1995) consider the fractional total mass lossk(φ1 ) and number loss consider the fractional total mass loss (φ1 ) and number loss (φ0 ) at time t which can be written as (φ0 ) at time t which can be written as Ik (0) − Ik (t) = loss Ik (0) Ik.(t) loss fractions 3φk (t) and−number φMass . k (t) = Ik (0) Ik (0) (12) (12) Note that we use the notation with numerical indices (since We assume that havewith a minimum mass of(since mthr Note that weice usecrystals the notation indices the expressions moments suggestnumerical it) interchangeably −3 ng). using (e.g. 10 Then we define for k ∈ {0, 1} the following thetheexpressions using suggest interchangeably with notation using (m,moments n) as indices (the it) notation that is with the notation using (m, as indices notation thatof is integrals which give the total number and(the mass fractions used in the quoted papers), i.e. n) the following identities hold: used in the quoted papers), i.e. the following identities hold: the ice mass distribution exceeding the threshold: φ0 ≡ φn , φ1 ≡ φm , I0 ≡ In , I1 ≡ Im (and correspondingly , φ1 ≡ φmbelow). , I0 ≡ Inφ,nI(φ I is (and correspondingly 0 ≡fkφn 1 ≡ for φthe introduced plotted in Fig. 2. m) m for the fk introduced below). φn (φm ) is plotted in Fig. 2. ∞ Z Ik (t) := mk f (m, t)dm. (11) mthr www.atmos-chem-phys.net/9/7481/2009/ 10 0.2 0.2 0 0 0 0 0.2 0.2 0.4 0.4 0.6 0.6 0.8 0.8 φm φm 1 1 Fig. Fig. 2. Total fraction of number loss, loss, φn ,loss, vs. fraction of 2. of of number φn ,φtotal vs. total fraction of of Fig. 2. Total Totalfraction fraction number total fraction n , vs. massmass loss, loss, φ for initialinitial geometric mean mean masses from 1from m, φ masses 1 1 mass loss, φmm,various ,for forvarious various initialgeometric geometric mean masses from to 1000 ng. Note that the curves are almost congruent. Time Time runs runs to ng. the areare almost congruent. to 1000 1000 ng. Note Notethat that thecurves curves almost congruent. Time runs alongalong the curves from (0, 0)(0, to (1, 1). 1). alongthe thecurves curvesfrom from (0,0)0)toto(1,(1, 1). TimeTime runsruns alongalong the curves fromfrom (0, 0) to 0) (1,to1).(1,We see the curves Wethat see that Since fis depends on time, so(0, doesnegligible Ik . 1). Harrington et al. initially there mass loss combined with num-numinitially there is mass loss combined with negligible (1995) consider the fractional total mass loss (φ ) and num1 ber loss, but the loss overhauls in theinlater phases of of ber loss, butnumber loss overhauls the later ber losssublimation (φ0 )the at number timeprocess. t which canisbewhat written as phases the ongoing This we expect for the ongoing sublimation process. This is what we expect for massmass distributions masses exceeding the threshIk (0)with − Iwith (t) mode distributions masses exceeding the threshkmode φk (t) Different = . can be expected for exponen(12) old mass. behaviour old mass. Different behaviour can be expected for exponenIk (0) tial distributions. We note that Harrington et al. (1995) also tial distributions. We note that Harrington et al. (1995) also Note that we usea the notation with numerical indices (since had examples with a different behaviour. had examples with different behaviour. Inthe a In cloud model, we generally do neither haveit) knowledge expressions using moments suggest interchangeably a cloud model, we generally do neither have knowledge of the initial values I (0) nor of the time t which must be in-be that with the notation using (m, n) as indices (the k of the initial values Ik (0) nor of the time t whichnotation must in- is terpreted here as the time passed by since sublimation started. used in the quoted i.e.by the following identities hold: terpreted here as the papers), time passed since sublimation started. (Since act inna, cloud model simultaneously it for the φ0many ≡φnmany , processes φ1 ≡φ Iin1 ≡I correspondingly m , I0 ≡Iact m (and (Since processes a cloud model simultaneously it would even make sense toφnintroduce such a time variable fknot introduced (φ ) is plotted in Fig. 2.variable Time runs would not even below). make sense tomintroduce such a time or toalong track the values). in 1). a model we that usu- initially the “initial” curves from (0, Hence, 0) toHence, (1, see or to track the “initial” values). inWe a model we usually can only consider the fractional mass and number loss therecan is mass loss combined with negligible ally only consider the fractional mass andnumber numberloss, loss but per time step, which can be written as the time number overhauls in the later per step,loss which can be written as phases of the ongoing Ik (t)process. − I (t + This ∆t) is what we expect for mass dissublimation Ik (t)k− Ik (t +.∆t) fk (t, ∆t) = (13) ftributions (t, ∆t) = . withImode masses exceeding the threshold(13) mass. k k (t) Ik (t) Different behaviour can be expected for exponential distriThese fractions depend on the size of the time step ∆t, but These fractionsnote depend the size of the step ∆t,had but exbutions. that on Harrington al. time (1995) still on the timeWe since sublimation started.etExamples foralso varstill on the time since sublimation started. Examples for varwith a different behaviour. ious amples time step values ∆t are plotted in Fig. 3: These curves stepmodel, values we ∆t generally are plotteddo inneither Fig. 3: have Theseknowledge curves Intime a{f cloud link ious pairs m (ti , ∆t), fn (ti , ∆t)} for times ti = i · ∆t link pairs {f (t , ∆t), f (t , ∆t)} for times t = m i n i i of the initial values I (0) nor of the time t which must be in(i = 1, 2, 3, . . .) running kuntil the ice is completely sub-i · ∆t (i = 1, 2, 3, . . .) running until the ice is completely subterpreted here as the time passed by since sublimation started. limated. (The yellow dot at (1, 1) was computed with a (The yellow atice 1) was computed with a it (Since many processes act a(1, cloud model simultaneously verylimated. large time step, such thatdot thein sublimated completely very large time step, such that ice sublimated completely within this single time step). Thetothe curves fn (fsuch ) all have would not even make sense introduce a time variable m within thisThey single time curves fmeans all have n (fm ) that similar nearstep). the fmThe –axis whichin or shape. to track the start “initial” values). Hence, a model we ususimilar shape. start near the fwithout which means that m –axis number the initial mass lossThey occurs alone ally can only consider thealmost fractional mass and loss, number loss the initial mass loss occurs alone almost without number loss, per time step, which can be written as fk (t, 1t) = Ik (t) − Ik (t + 1t) . Ik (t) (13) Atmos. Chem. Phys., 9, 7481–7490, 2009 4 7484 4 K. Gierens and S. Bretl: Analytical treatment of sublimation K. Gierens Gierensand andS.S.Bretl: Bretl: Analytical treatment of sublimation Analytical treatment of sublimation 0.0035 1 0.0035 1 0.003 0.003 0.8 0.0025 0.0025 0.8 f’f’nn 0.002 0.002 0.0015 0.0015 fn fn 0.6 0.6 0.001 0.001 0.4 0.4 0.0005 0.0005 0 0.2 00 0.2 0.0005 0.0005 0.001 0.001 0.0015 0.002 0.0025 0.003 0.0015 0.002 0.0025 0.003 f’m f’m fn0 n00vs. 0 0 0 0 0.2 0.2 0.4 0.4 0.6 fm0.6 0.8 0.8 1 1 fm Fig. 3. Mass loss (fm ) and number loss (fn ) fractions for series of time steps. are 100, 200, 300, Mass loss losssublimation (fm and number number (fnn)steps of Fig. 3.subsequent Mass (f lossTime (f fractions for series m)) and 400 s (solid red, green, blue, dashed red), and time runs 200, along300, each steps are 100, subsequent sublimation time steps. Time curve from the point neares to thered), fm –axis to the point nearest to red, green, blue, dashed and time runs along each 400 s (solid the f –axis. The individual time steps are marked on each curve. the point point neares neares to to the the ffmm -axis curve fromnthe –axis to to the the point point nearest to Arrows indicate the direction of time. The yellow point at (1, 1) was -axis. The individual time steps are marked on each curve. the fnnthe –axis. resultThe of aindividual test with a very long time step that should guarantee Arrows indicate the direction of time. The yellow pointThe at (1, 1) was that the ice sublimates completely within that step. black line 0.89 should guarantee the result a test with very is theofattempt of a fita of thelong later time parts step of thethat curves, fn =f m . The that step.is m The black that the ice geometric sublimatesmean completely initial mass for within the calculations ng. line 0 =1 0.89 fm is the attempt of aa fit fit of of the thelater laterparts partsof ofthe thecurves, curves,ffnn==f m . The = 1 ng. ng. initial geometric mean mass for the calculations is m m00 =1 and after about 600 s they reach an “attractor” that can be apα̃ proximately be fitted by fn = fm with α̃ = 0.89. α̃ < 1 again signifies that later in the sublimation thebenumandThese after about 600depend s they reach an size “attractor” that apfractions on the of theprocess timecan step 1t, α̃ of the curves shows that fn ber loss catches up. The shape proximately be fitted fn sublimation = fm with started. α̃ = 0.89. α̃ < 1 but still on the time by since Examples issignifies not reallythat function the mathematical of fnumm beagain later in(in the sublimation the for various time astep values 1t are plottedprocess insense) Fig. 3: These cause it is not unique even if the timestep is fixed. This makes ber losslink catches The shape ofi ,the curves shows that fn curves pairs up. {f (t fn (t 1t)} for times ti = i · 1t i , 1t), it questionable m whether a functional dependence for parameis not1,really a. function (inuntil the mathematical sense) of fsubli(i = 2, 3, . .) running the ice is completely m beterisation of sublimation should be used in bulk models. cause is(The not unique even the(1, timestep is computed fixed. This makes mated.it The yellow dotifat a timestep dependence of 1) fk was suggests a Taylorwith expanit questionable whether a functional dependence for paramevery large time step, such that the ice sublimated completely sion which yields terisation sublimation should be used in bulk models. within thisofsingle time step). The 2 curves fn (fm ) all have simfktimestep (t, ∆t) =dependence fk0 ∆t + O(∆t ). suggests a Taylor expan(14) ilarThe shape. They start near theoffmfk–axis which means that the As Fig. 3 shows, the higher orders cannot be neglected at sion initialwhich massyields loss occurs alone almost without number loss, time steps of the order 100 s and longer. Hence the following after about 600 they 2reach an “attractor” that can(14) be fand ∆t) = fisk0 ∆t + sO(∆t ). k (t, analysis strictly valid models with approximately be fitted by only fn =for fmα̃cloud withresolving α̃ = 0.89. α̃ < 1 small time steps of higher the orderorders seconds (wherebetheneglected order As Fig. 3 shows, cannot at again signifies thatthe later in the sublimation processhigher the numterms of arethe negligible), but it might still give some guidance time steps order 100shape s and longer. Hence the following ber loss catches up. The of the curves shows that fn for the treatment of sublimation in large–scale models. analysis is strictly valid(in only for cloud resolving models is not really a function the mathematical sense) of fmwith beFirst, we have small time steps of the order seconds (where the higher order cause it is not unique even if the timestep is fixed. This makes dIkstill (t) give some guidance ∂f ∆t) k (t, terms are negligible), it−1 might it questionable whether a=functional dependence for parame= fk0 (t)but , (15) ∂∆t Ik (t) in dt for the treatment of sublimation terisation of sublimation should be large–scale used in bulkmodels. models. 0 First, we still haveretains the timeof dependence. Weanote that 1/f Thewhich timestep dependence fk suggests Taylor expank (t) can be yields interpreted as−1 a timescale sion which dIk (t) for the change of the cor∂fk (t, ∆t) = fk0 (t) = , (15) ∂∆t Ik (t) 2 f (t, 1t) = f 0 1t + O(1t ). dt (14) k 0 k which still retains the time dependence. We note that 1/fk0 (t) 3 shows,asthea higher orders cannot be neglected at canAsbeFig. interpreted timescale for the change of the cortime steps of the order 100 s and longer. Hence the following Atmos. Chem. Phys., 9, 7481–7490, 2009 0 0 for fm m 0 initial geometric mean masses from from 1 Fig. Fig. 4. 4. f vs. f forvarious various initial geometric mean masses 1 for various initial geometric mean masses from 1 vs. fm red, Fig. 4. ng fng n (dashed to 1000 solid green, blue, red).red). NoteNote that the inverse to 1000 (dashed red, solid green, blue, that the inverse to 1000of (dashed red, solidtogreen, blue, red).forNote inverse values the axis thethe timescales the change of values ofng the axiscorrespond correspond to timescales for that the the change of values of the axis correspond to the timescales for the change of the corresponding integrals I (t) in seconds. Arrows indicate the the corresponding integralsk Ik (t) in seconds. Arrows indicate the direction of time. integrals Ik (t) in seconds. Arrows indicate the the corresponding direction of time. direction of time. responding integral. The derivatives of the integrals can be analysis is strictly valid only for cloud resolving models with computed in the following responding integral. Theway: derivatives of the integrals can be small time steps of the order seconds (where the higher order computed Z∞ in the following terms but itway: might still give some guidance dIk are negligible), k ∂f = m · dm, (16) for the treatment of sublimation in large-scale models. ∞ Z dt ∂t dI ∂f k First, we have =mthr mk · dm, (16) dt (t, 1t) ∂t −1 dI (t) ∂f andk the m partial derivative of the mass distribution function is: k 0 thr = fk (t) = , (15) ∂1t Ik (t) dt ∂f and = thef × partial derivative of the mass distribution function (17) is: which still retains the time dependence. We note that 1/fk0 (t) ∂t ∂f be interpreted as a timescale for the change of the corcan = f× (17) ∂t ³integral. responding The ´derivatives of the integrals can be 1−b m −(1−b)at a b 1−b computedlnin the following way: (1 − b)am m0 + . 2 [m1−b − (1´ ³ σ ) − b)at] m − (1 − b)atmb (1 − b)(ln m ∞ 1−b Z m −(1−b)at a ln dIk ∂f 1−b (1 − b)amb(16) 0 = 0 mk · mdm, + . 0 dtf(1 ∂t 2 1−b fm isσplotted in Fig. 4. − These n vs. −mb)(ln − (1 b)at]curves mlook − (1similar − b)atmb m ) [m to those inthrFig. 3, and indeed they are equivalent to those for aand unitthe time step of 1 s. partial derivative of the mass distribution function is: 0 fn0 vs. fm is plotted in Fig. 4. These curves look similar to those in Fig. 3, and indeed they are equivalent to those for 4a∂funit Time scales time step of 1 s. = f× (17) ∂t curves φ The (φ ) in Fig. 2 look very similar for different n m m1−b −(1−b)at initial mean masses, but if we would include tick marks for ln a 4 Time scales m1−b b (1 − b)am 0 time along the curves they would differ for different curves. + . m −with (1 −respect b)atmb (1can − b)(ln )2try [m1−b − (1 these − b)at] We therefore to unify functions The curves φσnm(φ m ) in Fig. 2 look very similar for different to time as well by introducing a dimensionless time τ . The initial mean masses, but if we would include tick marks for corresponding τ –tick marks would then become nearly contime the curves they would differcurves for different curves. fn0 along vs.For fm0this is plotted 4. These look similar gruent. we can in firstFig. compute the time T it needs to to We can therefore try to unify these functions with respect those in Fig. 3, and indeed they are equivalent to those sublimate completely (i.e. to mass zero) a crystal having ex- for a to time wellm a dimensionless time τof. The unit time step ofby s.introducing actly theas mass , which can be any characteristic mass 01 corresponding τ –tick marks would then become nearly the chosen distribution, (for instance the median, mean, or congruent. For this we can first compute the time T it needs to 4sublimate Time scales completely (i.e. to mass zero) a crystal having exactly the mass m0 , which can be any characteristic mass of look verythe similar for mean, different The curves distribution, φn (φm ) in Fig. the chosen (for2 instance median, or initial mean masses, but if we would include tick marks for www.atmos-chem-phys.net/9/7481/2009/ K.K.Gierens Gierensand andS.S.Bretl: Bretl:Analytical Analyticaltreatment treatment of of sublimation sublimation www.atmos-chem-phys.net/9/7481/2009/ 1.4 1.2 1 0.8 h(τ) mode mass). wethey takewould for m0differ the geometric mean mass time along the Here curves for different curves. of can the chosen log–normal distribution. This timewith is respect We therefore try to unify these functions to time as well by introducing a dimensionless time τ . The m1−b 0 corresponding τ -tick marks would then become nearly conT = . (18) − b)we can first compute the time T it needs to gruent.|a|(1 For this sublimate (i.e. to τmass zero) With thiscompletely time we introduce as t/T , i.e.a crystal having exactly the mass m0 , which can be any characteristic mass of (b−1) the chosen or τ= t|a|(1distribution, − b)m0 . (for instance the median, mean,(19) mode mass). Here we take for m0 the geometric mean mass the dimensionless time variable ofHence, the chosen log-normal distribution. Thistakes timeinto is account the chosen initial characteristic mass of the mass distribution 1−b and themcurrent sublimation rate. It does not take into account 0 T other = quantities . like the width of the mass distribution. (18) We |a|(1 − b) define With this introduce t/T , i.e. f 0 time (a, mwe d ln Iτnas (τ )/dτ 0, τ ) h(τ ) = n0 = . (20) f (a, m(b−1) , τ) d ln Im (τ )/dτ τ = t|a|(1 m − b)m00 . (19) h(τ ) can be interpreted as the ratio of two timescales for Hence,of thethe dimensionless variable takes and into their account change Ik integrals. time These timescales rathe massinofFig. the 5mass tiochosen vary ininitial time.characteristic h(τ ) is plotted for distribution various iniand current sublimation It does not take tialthe geometric mean massesrate. (from 1 to 1000 ng)into andaccount various other quantities likeWe thecan width of thethemass distribution. We sublimation rates. observe following behaviour: define up to a normalised time τ ≈ 0.1 sublimation leads almost only tofa0 (a, mass m0loss , τ ) and dthe ln number In (τ )/dτdensity of the ice crysn h(τ )= (20) = Number loss. commences at about tals stays0 nearly constant. f (a, m , τ ) d ln Im (τ )/dτ τ ≈ 0.1 mand the0fractional number loss rate exceeds the fractional massbeloss rate (h >as1)the at about τ ≈ and thereafter, h(τ ) can interpreted ratio of two1 timescales for that is,ofonce characteristic mass had sufficient time to change the Ithe integrals. These timescales and their rak completely. shapeinofFig. a curve h(τvarious ) depends on tiosublimate vary in time. h(τ ) isThe plotted 5 for initial the widthmean (and shape) the initial massng) spectrum. The trangeometric massesof(from 1 to 1000 and various subsition from mass loss to number loss regime is sudden limation rates. We can observe the following behaviour:forupa distribution gradual for a broad one (not shown). tonarrow a normalised time and τ ≈0.1 sublimation leads almost only to However, as long as we chose a fixed value for σm (as in the a mass loss and the number density of the ice crystals stays figure), all these functions are very similar and they can be nearly constant. Number loss commences at about τ ≈0.1 fitted with a generalised log–logistic function: and the fractional number loss rate exceeds the fractional mass loss rate (h>1) ψ at about τ ≈1 and thereafter, that is, ³ ´¡ ¢ . h̃(τ ) = (21) p had sufficient time to sublimate once the characteristic p+1 0 1 + p−1 τmass τ completely. The shape of a curve h(τ ) depends on the width (and of the is initial The transition from Theshape) formulation suchmass that τspectrum. 0 is the inflexion point of the mass loss to number loss regime is sudden forwell a narrow fit function. The latter is plotted in Fig. 5 as with ψdis= tribution and gradual for a broad one (not shown). 1.24, p = 2.4, τ0 = 0.3. ψ is the asymptotic valueHowever, of the fit asfor long as we chose value unity for σm (as inisthe figure), all large values of τa.fixed It exceeds which an expression these functions are very similar and they can be fitted with a for our earlier finding that in the end the number loss exceeds generalised log–logistic the mass loss rate. The function: parameter p controls the steepness of the fit around the inflexion point, i.e. it measures how fast ψ sublimation loss changes from . the mass loss to the number (21) h̃(τ )= p+1the inflexion τ0 p regime.1 Finally, point is found here at 0.3 which + p−1 τ means that the transition into the number loss regime occurs at a considerably shorter time than is needed to sublimate a The formulation is such that τ0 is the inflexion point of crystal with the chosen characteristic mass. the fit function. The latter is plotted in Fig. 5 as well with We see that it is possible to find a certain universal beψ = 1.24, p = 2.4, τ0 = 0.3. ψ is the asymptotic value of haviour of the sublimation curves that do not depend on inithe fit for large values of τ . It exceeds unity which is an tial mean mass or sublimation rate. The function does howexpression forwhen our earlier that in the enddistributions, the number ever change we usefinding different initial mass loss exceeds the mass loss rate. The parameter p controls the steepness of the fit around the inflexion point, i.e. it measures 7485 5 0.6 0.4 0.2 0 0.01 0.1 1 10 τ Fig. 5. 5. h(τ h(τ) )vs. vs.dimensionless dimensionlesstime timeτ τfor forvarious variousinitial initial geometric Fig. geometric mean masses massesand andsublimation sublimationrates: rates: 1 ng, a= −0.04(red); (red); mean m0m=1 a= −0.04 0 =ng, m00 = 10 ng, aa = = −0.09 (green); (green);mm = 100ng, ng,a = a =−0.2 −0.2(blue); (blue); m =10 0 0=100 m ng, aa==−0.5 −0.5 (violet).These These curves similar m00 ==1000 1000 ng, (violet). curves areare so so similar that that be seen. dashed black a generalized onlyonly one one can can be seen. TheThe dashed black lineline is aisgeneralized log– log–logistic function logistic function thatthat fits fits h(τh(τ ). ). e.g. to achanges differentfrom σm (not shown). how by fastchanging sublimation the mass loss The to themain numproblem still thatFinally, the valuethe of inflexion h dependspoint on theistime since ber loss isregime. found here sublimation not have into this the information at 0.3 whichstarted. means As thatwe thedotransition number in loss cloud know easily whether process is regimemodels occurswe at cannot a considerably shorter timethe than is needed still in the phase where mass is much larger than the to sublimate a crystal with the loss chosen characteristic mass. number lossthat (τ < or already theaphase where numberbeWe see it 0.1) is possible to in find certain universal loss catches up sublimation (τ > 1) or somewhere between (τ close haviour of the curves thatindo not depend on to inithe point). tial inflexion mean mass or sublimation rate. The function does howIt is clear that τ0 ordistributions, τ = 1 is ever change whenthe wetime use corresponding different initialtomass ae.g. characteristic timetoofa the sublimation process. It might be by changing different σm (not shown). The main useful to know it for practical applications that we consider problem is still that the value of h depends on the time since next. For the started. parameters in Fig. 5 the this timeinformation scales range in sublimation As used we do not have from 40 to 250 s, that is, time steps of cloud resolving models is cloud models we cannot know easily whether the process are mostly smaller than the characteristic times, while thosethe still in the phase where mass loss is much larger than of climate models are often larger. number loss (τ <0.1) or already in the phase where number loss catches up (τ >1) or somewhere in between (τ close to the inflexion point). 5 ItTests of parameterisations in two–moment models τ = 1 is a is clear that the time corresponding to τ0 or characteristic time of the sublimation process. It might be In the foregoing sections we have seen that it is necessary useful to know it for practical applications that we consider to know the time since sublimation started when its effect on next. For the parameters used in Fig. 5 the time scales range the number and mass concentrations is to be treated correctly, from 40 to 250 s, that is, time steps of cloud resolving models and the the problem is just that this time cannot be defined are mostlyonce smaller the characteristic while those generally otherthan processes act in a cloudtimes, as well. of climate models are often larger. In a two–moment model one needs both quantities, fn and fm . It is easier to formulate an equation for fm than for fn because is an analytic equation for the mass change 5 Teststhere of parameterisations in two-moment modelsof single crystals, while there is none such for the number (it is either or one,sections which iswe non–analytic in the In thezero foregoing have seen that it mathematis necessary ical sense). A formulation for fm can be when made its in effect a rela-on to know the time since sublimation started tively straightforward once the current mass spectrum is the number and mass way concentrations is to be treated correctly, known assumed. Weishave sublimation and theorthe problem just seen that in thisSect. time2 how cannot be defined generally once other processes act in a cloud as well. Atmos. Chem. Phys., 9, 7481–7490, 2009 changes the shape of the mass spectrum. is ignored in In a two-moment model one needs both This quantities, fn and such that errors arise mass ftwo–moment to formulate an equation forinfmthethan forloss fn m . It is easiermodels, computation well as in the number (as we because there as is an analytic equation forloss the fractions mass change of will see below). single crystals, while there is none such for the number (it Therezero are or twoone, principle to parameterise subis either which possibilities is non-analytic in the mathematlimation in two–moment models, either one defines f as a ical sense). A formulation for fm can be made in an reladirect function of f or one formulates f independently m way once the current n mass spectrumof tively straightforward is f . The second approach is a bit risky, it does not m known or assumed. We have seen in Sect. 2 since how sublimation guarantee fn = for spectrum. fm = (0, 1), so is that a mixed changes thethat shape of (0, the 1) mass This ignored in approach that gives this guarantee would perhaps be prefertwo-moment models, such that errors arise in the mass loss able. Whenasfnwell is aasdirect fm ,fractions the power computation in thefunction numberofloss (as law we α is the simplest formulation that fulfills f = (0, 1) f = f n n will see m below). for fm =are (0,two 1). principle possibilities to parameterise subThere In the following we test a number potential limation in two–moment models, eitherofone definesformulafn as a tions. The tests are all based on the corresponding “benchdirect function of fm or one formulates fn independently of functions φn (φm ) obtained from the analytical solufmark” m . The second approach is a bit risky, since it does not tion derived in fSect. 2, see Fig. 2. That is, we take a formulaguarantee that n = (0, 1) for fm = (0, 1), so that a mixed tion of f , and compute the corresponding functionbeφprefern n (φm ) approach that gives this guarantee would perhaps up to complete sublimation and compare the result to the able. When fn is a direct function of fm , the power law benchmark φ (φm ). The tests use the following algorithm: fn = fmα is then simplest formulation that fulfills fn = (0, 1) for1.fmStart = (0,loop 1). over time steps; In the following we test a number of potential formulations. The testsmass are change: all baseddM on ∝ theaµ corresponding “bench2. compute b dt; mark” functions φn (φm ) obtained from the analytical solucompute change: fmis,=we −dM/M ; 2. That take a formulation3.derived in relative Sect. 2, mass see Fig. tion of fn , and compute the corresponding function φn (φm ) 4. compute number change (various methods, see below: up to complete sublimation and compare the result to the e.g. fn = f α → dN = −fn N or dN ∝ aµb−1 dt); benchmark φn (φmm). The tests use the following algorithm: 5. update mass and number, update mode mass for f (m), 1. Start loop over time steps; output of various quantities; 2.6. compute change: 1M ∝ aµb 1t; end timemass step loop. 3. compute relative mass change: fm = −1M/M; 5.1 Power laws 4. compute number change (various methods, see below: α A first exampleαshowing a test of fn = fm α = 1.1 e.g. fn = fm → 1N = −fn N or 1N∝aµwith b−1 1t); (Spichtinger and Gierens, 2009) is given in Fig. 6. We see that the parameterisation produces too high lossf frac5. update mass and number, update modenumber mass for (m), tionsoutput in theofearly phases of sublimation while in the final various quantities; phase the mass loss fractions are overestimated relative to 6. number end timeloss. stepObviously, loop. the a choice of α < 1 would deteriorate the situation, and a much larger value of α would only 5.1 Power improve the laws agreement for the initial phase of sublimation at the price of much worse results in the later phases. α A first example a test n = fphase m with One could try toshowing use a large α in of the finitial andαα=<1.1 1 (Spichtinger and Gierens, 2009) is given in Fig. 6. We see later. The problem is, however, that one cannot decide in that produces toothe high number loss fracthe the bulkparameterisation cloud model in which phase sublimation process tions in the early phases of sublimation while in the finala is, as we have seen in the foregoing sections. Thus, such phase the mass loss fractions are overestimated relative to possibility is not given. the number loss. Obviously, a choice of α<1 would deteriorate situation, and a much larger value of α would only 5.2 the Other functions improve the agreement for the initial phase of sublimation at Weprice tested relations fn and fm as the of other muchfunctional worse results in thebetween later phases. well, particular give a zero derivative fm α<1 =0 Oneincould try to such use athat large α in the p initial phaseatand α with α > 1 1− fm (not shown). Examples are fn = that 1 − one later. The problem is, however, cannot decide in the bulk cloud model in which phase the sublimation process Atmos. Chem. Phys., 9, 7481–7490, 2009 K. K. Gierens Gierens and and S. S.Bretl: Bretl: Analytical Analyticaltreatment treatmentofofsublimation sublimation 1 0.9 0.8 0.7 0.6 φn 6 7486 0.5 0.4 0.3 0.2 0.1 0 0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 φm 1 Fig. Fig. 6. 6. φφnn vs. vs. φ φm as parameterized parameterized inin Spichtinger Spichtingerand andGierens Gierens m ,, as (2009) (2009) (red (redlines, lines,for forvarious variouschoices choicesofofsublimation sublimationrates ratesand andinitial initial geometric geometric mean meanmasses), masses),compared comparedwith withthe theanalytical analyticalsolution solutionfor for various various initial initial geometric geometricmean meanmasses massesand andsublimation sublimationrates rates(black (black line). line). Only Only one one black blackline linecan canbe beseen seenbecause becausethe thedifferences differencesbebetween tween the the analytical analyticalsolutions solutionsare aresmaller smallerthan thanthe thethickness thicknessofofthe the curve. curve. and = have [cos((f + 1]/2. This did not yieldsuch real a m − is, asfnwe seen in 1)π) the foregoing sections. Thus, improvements over the simple power law. In these cases, possibility is not given. φn ≈ 0 until most of the ice mass is sublimated (unless α is very to functions one). 5.2 close Other 5.3 Usingother maximum sublimating crystal massfn and fm as We tested functional relations between well, in particular such that give a zero at fm = 0 p derivative Alternatively can compute the maxα 1−fmodel (not shown). one Examples are fnin = the 1− cloud m with α>1 and imum crystal mass mmax that sublimates within a timestep. fn = [cos((f m −1)π )+1]/2. This did not yield real improveAssuming the Koenig is cases, given as ments over the simpleapproximation power law. In this these φn ≈0 until 1/(1−b) most of the ice mass is sublimated (unless α is very close m = (|a|∆t) . (22)to max one). With this quantity at hand we can compute R mmaxmaximum sublimating crystal mass 5.3 Using f (m) dm fn = 0R ∞ , (23) Alternatively onedm can compute in the cloud model the maxf (m) 0 imum crystal mass mmax that sublimates within a timestep. while fm isthe computed by the model in theis usual Assuming Koenig approximation this given way. as For the calculation of the numerator integral we may use expres1/(1−b) sions truncated moments when analytical expressions for mmax for = (|a|1t) . (22) them are available. For our special choice of a log–normal With this quantity hand we can compute distribution we haveat(cf. Jawitz, 2004): R ¸ Z mmax mmax f (m) dm · ln(mmax /m0 ) 1 1 fn = R0f∞ , (23) √ + (24) (m) dm = erf 2 ln σm 2 0 0 f (m) dm2 It turnsfout that this method produces for too while computed by the modelbad in results the usual way.large For m is and too small time steps. For toointegral large time stepsuse (even 1s the calculation of the numerator we may expressions for truncated moments when analytical expressions for www.atmos-chem-phys.net/9/7481/2009/ K. Gierens and S. Bretl: Analytical treatment of sublimation 7487 them are available. For our special choice of a log–normal distribution we have (cf. Jawitz, 2004): Z mmax 1 1 ln(mmax /m0 ) f (m) dm = erf + (24) √ 2 2 ln σm 2 0 sinusoidal oscillation. The sublimated ice is assumed to add to the water vapour, i.e. to increase the relative humidity. The initial conditions are chosen such that we start with ice saturation and if we would completely sublimate the ice we would reach RHi = 105%. The oscillation amplitude is assumed to be ±5%, as well. Hence we have: It turns out that this method produces bad results for too large and too small time steps. For too large time steps (even 1 s turned out too large for m0 = 1 ng and a = − 0.04) fn is non-zero at the beginning, and for too short time steps (0.1 s) we have again the problem that φn ≈ 0 until most of the ice mass is sublimated. 5.4 Using moments Another possibility one could think about is to formulate fn in a cloud model via the moments of the mass distribution. These are defined as Z ∞ µk = mk f (m) dm. (25) 0 Spichtinger and Gierens (2009) use dqc /dt = aµb (corrections neglected) to calculate the tendency of the ice mixing ratio from which fm is computed. In analogy, we may set dN/dt = aµb−1 to calculate the tendency of the number mixing ratio and compute fn from it. (Although µb−1 is a moment of negative order, it works since the corresponding integral is finite). Although this sounds a logical approach, it is not. In this case we have fm0 = − aµb /µ1 and fn0 = − aµb−1 /µ0 , which shows that h(τ ) turns out as a constant (since the time dependent mode mass cancels out in the division fn0 /fm0 and σm is constant). This is not only in contradiction to the analytical behaviour of h(τ ) (Fig. 5), but – even worse – it also implies fn = cfm (c a constant) which violates the boundary conditions at (1, 1), unless c = 1, which it is generally not since it depends on b (pressure and temperature dependent) and σm . 5.5 Effect of humidity fluctuations around ice saturation Finally we test the effect of small–scale humidity fluctuations around ice saturation (caused by random fluctuations or atmospheric waves) on sublimation. Such a situation can arise in old contrails or cirrus clouds (where relative humidity had enough time to equilibrate with the ice crystal ensemble) under certain synoptic conditions, namely when the large–scale vertical wind is very weak (less than a few cm s−1 ). Since a is a non–explicit function of time in such a case, the analytical solution is no longer valid and also the more general solution of Appendix A is not applicable. Hence we choose a simple numerical procedure. We divide the lognormal mass distribution in 1000 discrete initial masses, compute the mass growth/sublimation rates for each mass with 1 s timesteps. Once a mass gets smaller than a threshold of 0.001 ng, it is assumed to be lost. The fluctuations are represented with a www.atmos-chem-phys.net/9/7481/2009/ RHi = 100 − 5 sin(2π ωt) + 5φm (%). (26) Note that φm can become negative in the growth phases. We use a geometric mean mass of 100 ng. At RHi = 95% (220 K, 250 hPa) we get a = − 9.1×10−4 , the characteristic time (i.e. τ = 1) is 5800 s. The oscillation frequency chosen was ω = 1/250 s−1 , which is a typical value for a BruntVäisälä oscillation in stably stratified air. A first test of the numerical method with constant subsaturation gave φn (φm ) as in Fig. 2 which shows that the numerical procedure works well. When we switch on the oscillation and add the sublimated ice to the relative humidity both mass and number loss are reduced strongly; after 30000 s simulation time only a few percent of the mass and less than one per mille of the number are lost. With a lower frequency of ω = 1/2500 s−1 (gravity wave) these numbers are larger, because the initial sublimation period lasts much longer, but still less than 10 percent of the number is lost after 30 000 s. The results can be explained as follows: Initially the mean relative humidity is ice saturation, but the sublimating ice adds to this mean, such that quickly a new mean value is achieved that exceeds saturation. Hence, in spite of the oscillations that always lead transiently through subsaturated states, on the average the sublimation process is halted. After the first sublimation period all crystals that were small enough for sublimation are lost, but in the following sublimation phases the remaining crystals are large enough to survive. Unfortunately, a different behaviour is displayed by a model employing the simple parameterisation fn = fmα . Here, more than 20% of the ice is lost within 30 000 s and with ω = 1/250 s−1 , while the ice mass stays approximatly constant. This is obvioulsy the effect of adjusting the mass distribution after each time step to a new log-normal distribution (with changed geometric mean mass). Hence although the small crystals are gone within the first sublimation phase, there are new small crystals in the next, merely because the fixed distribution type enforces this. This leads to crystal loss in every new sublimation phase. This means that under conditions of a cloud in equilibrium (i.e. RHi ≈100%) small scale fluctuations in the cloud model can lead to an artificial crystal loss with corresponding consequences on further microphysical evolution and optical properties. 6 Discussion Having performed the simple tests of the various possible parameterisations we see now clearer the difficulties inherent in modelling ice sublimation in the framework of two-moment Atmos. Chem. Phys., 9, 7481–7490, 2009 7488 K. Gierens and S. Bretl: Analytical treatment of sublimation models. These difficulties arise in the same way when another mass distribution is chosen (we have also tested a generalised gamma distribution). An exponential distribution which is typical for cloud droplets could give different test results; this has not been tested in this paper because we are mainly interested in improvement of cirrus and contrail models. But such tests could be done in an analogous manner. As a general rule of thumb the analytical solutions showed that over a large fraction of the sublimation phase the number loss fraction equals roughly the mass loss fraction, as seen for instance in Figs. 2 and 3. In particular for large-scale models with long timesteps of the order of the sublimation timescale it seems therefore reasonable to set fn = fm . For cloud resolving models which need timesteps much shorter than the sublimation timescale problems can arise, in particular in the beginning of the process, when the number concentration is hardly affected although the mass concentration is already diminishing. Hence it is not easy to find a better parameterisation for a small-scale model. The simple parameterisation fn = fmα with α & 1 seems to obey the simple rule, but in the oscillation case it went wrong although the more exact simulation showed that the rule is valid in this case as well. Unfortunately, the oscillation case is not so academic like the other tests we have performed; we even took into account that the sublimating ice mass contributes to the vapour phase and thus to the relative humidity in the cloud. The oscillation case is typical for mature clouds where crystals have consumed the excess vapour completely and where random fluctuations (turbulence) and atmospheric waves of various kind affect the cloud evolution. In order to avoid artificial number concentration loss in such quasi-equilibrium cases one could either employ a larger value of α, such that larger mass loss is needed before crystal loss commences. Or one could introduce a sublimation humidity threshold of several percent below saturation. Both strategies have their disadvantages. A sublimation threshold several percent below 100% is unphysical and may have unforeseeable effects. Larger α underestimates crystal loss in situations of steady substantial sublimation (as do other functional relations, as we have seen); however, one can let α depend on the degree of subsaturation, with larger values at small and smaller values at larger saturation deficits. This has been tested as well and it produces better results than the parameterisation with constant α. The question arises whether there are other pieces of information available at timestep level in the two-moment model. We have: two independent moments, namely number and mass concentrations, and direct functions of them (all other moments, effective sizes, and so on). More information can only be provided by the thermodynamic state at the timestep, i.e. the relative humidity and the temperature. These quantities allow to additionally compute the maximum mass that can evaporate within one timestep. However, we have seen that even with this additional information it is difficult to construct a better parameterisation of sublimation; at least our approach in the previous section was not successful although it sounded plausible. Our analytical tests were admittedly a bit academic. The analytical solution is only valid for constant a, which would mean that sublimated ice would disappear from the system. In reality, the sublimating ice increases the vapour concentration which generally will lead to increasing a. Also the sublimation process was considered in isolation, which is reasonable for testing, but in reality other processes act simultaneously. The sublimation timescales can be very long especially when the subsaturation is low. In such a case, however, there may well be other processes with shorter timescales that then dominate the cloud evolution rendering the problems with sublimation less important. When subsaturation is larger or the mean mass smaller, sublimation time scales get shorter; then the sublimation process will quickly evolve into that regime where fn ≈fm , such that the problems with the initial phases lasts for a shorter period of time. Here it would turn out disadvantagous to have a larger α or one of the other approaches discussed in the previous section, because they lead to underestimation of the number loss over a large fraction of the whole sublimation process. Considering these arguments we think that, in spite of its weaknesses, the simple approach fn = fmα with α slightly exceeding unity or dependent on the degree of subsaturation (or unity for large-scale models) is still one of the best choices one can make. Atmos. Chem. Phys., 9, 7481–7490, 2009 7 Conclusions The analytic solution of the spectral form of the equation for deposition/sublimation and its application to ice sublimation gave the following insights: – The relation between fractional number loss and fractional mass loss is non-unique, that is, it is no function. However it seems advantageous to formulate it as a function in parameterisations of ice microphysics for both large-scale and small-scale models. – Sublimation timescales are usually longer than timesteps of cloud resolving models, and often but not generally shorter than timesteps of large-scale models. The latter case is easier to parameterise than the first one. – As a rule of thumb the analytical solutions showed that over most of the sublimation process the number loss rate equals approximatly the mass loss rate. It is therefore a good idea to set them equal in large-scale models with long timesteps (say, 15 min. and more). – For small-scale models (e.g. cloud–resolving and large– eddy models) we have tested a number of alternatives to the standard power law, but the power law turned out www.atmos-chem-phys.net/9/7481/2009/ K. Gierens and S. Bretl: Analytical treatment of sublimation 7489 to produce the best results compared to the analytical solution. being the antiderivative of a(t) (for constant a, A = at as in the main part of the paper). Now take the following viewpoint: Let m(0) be a random variable with a given probability distribution f0 [m(0)], e.g. the log–normal. Then the solution above (Eq. A2) effects a mapping from the random variable m(0) to the random variable m(t), that is unique (and invertible) over a certain interval in time, [0, T ], depending on the time dependence of a. Over this intervall it is possible to compute the probability distribution of m(t), ft [m(t)], using the substitution rule, i.e. – Care has to be taken with the power law formulation when a cirrus cloud or condensation trail at ice saturation undergoes small–scale humidity fluctuations (probably irrelevant for large–scale models). Without any counter–measure the power law with α close to one leads to severe overestimation of crystal loss. It might be better to let α be a function of saturation deficit with larger values at low deficit and values closer to one at larger subsaturations. The academic test cases of the present paper can only give insight about the problems inherent in parameterisations of ice sublimation. The success of an alternative parameterisation in “every day work” should, however, be checked against spectrally resolving microphysics models where sublimation acts in combination and in competition with all other processes. The analytical solution points to the very core of the problem: the sublimation process requires an additional parameter for the complete description of the mass spectrum. The additional parameter must be obtained from an additional equation which is difficult to formulate in general once a variety of other processes affect the shape of the spectrum as well. To introduce such new equations is probably not the best way to overcome the problems since this would add a significant amount of complexity to the bulk models. If exact solutions are required one should resort to bin models which do not suffer from the mentioned problems. Nevertheless, bulk models are useful and needed whenever there are computer time and memory constraints, which is a common situation. Therefore, in spite of the problems, we encourage their use, provided that their limits are thoroughly checked. Appendix A Solution of the spectral growth equation A more general analytic solution of the spectral growth equation that handles for instances cases with time dependent a(t) (but with constant b) is possible proceeding from the following point of view. Let dm = a(t) mb , dt (A1) then the solution of this nonlinear differential equation is m(t)1−b − m(0)1−b = (1 − b)A(t) (A2) with Z A(t) = t a(t 0 ) dt 0 0 www.atmos-chem-phys.net/9/7481/2009/ (A3) ft [m(t)] = f0 {m(0)[m(t)]} dm(0) dm(t) and the derivative is b dm(0) (1 − b)A(t) 1−b . = 1− dm(t) m(t)1−b (A4) (A5) ft [m(t)] is the desired solution of the spectral growth equation. For the special case b = −1 (radius growth equation for liquid droplets) formally identical solutions have been obtained using another method (seemingly going back to Sedunov, 1974) by Brenguier (1991, eq. 2.5). Appendix B Notation parameters in Koenig’s crystal growth parameterisation A time integral of a (Appendix A) f (m, t) time dependent ice crystal mass spectrum f0 ≡ fn number loss fraction per timestep f1 ≡ fm mass loss fraction per timestep g(x, t) transformed time dependent ice crystal mass sprectrum g̃(x − at) characteristic solution for g(x, t) h(τ ) time dependent ratio of time scales for number and mass loss I0 ≡ In total integrated number loss I1 ≡ Im total integrated mass loss m mass of a single ice crystal ṁ mass growth rate of a single ice crystal m0 characteristic mass of the spectrum or geometric mean mass N ice number mixing ratio p fit parameter (steepness of the transition from the mass loss to the number loss regime) qc ice mass mixing ratio RHi relative humidity with respect to ice t time since sublimation started T time required to completely sublimate crystal of characteristic mass; length of time interval (Appendix A) x transformed crystal mass a, b Atmos. Chem. Phys., 9, 7481–7490, 2009 7490 ẋ x0 α α̃ 1t µk φ0 ≡ φn φ1 ≡ φm σm σx ω K. Gierens and S. Bretl: Analytical treatment of sublimation transformed mass growth rate transformed geometric mean mass power law exponent for the sublimation parameterisation fit parameter model time step moment of order k total fractional number loss total fractional mass loss geometric standard deviation of mass spectrum geometric standard deviation of transformed mass spectrum oscillation frequency Acknowledgements. We are grateful to Johannes Hendricks for critically reading a preliminary version of the manuscript and to Peter Spichtinger for providing a piece of software that we could use for the numerical exercise. The comments of two reviewers helped to improve the paper. The results of the work contribute to the development of two-moment ice physics schemes in the framework of the DLR project CATS. Edited by: J. Quaas References Brenguier, J. 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