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ALMA chemical survey of disk-outflow sources in Taurus (ALMA-DOT). IV. Thioformaldehyde (H$_2$CS) in protoplanetary disks: spatial distributions and binding energies

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Aims: To trace the radial and vertical spatial distribution of H2CS, a key species of the S-bearing chemistry, in protoplanetary disks. To analyse the observed distributions in light of the H2CS binding energy, in order to discuss the role of thermal desorption in enriching the gas disk component. Methods: In the context of the ALMA chemical survey of Disk-Outflow sources in the Taurus star forming region (ALMA-DOT), we observed five Class I or early Class II sources with the o-H2CS(7_1,6-6_1,5) line on a 40 au scale. We estimated the binding energy (BEs) of H2CS using quantum mechanical calculations, for the first time, for an extended, periodic, crystalline ice. Results: We imaged H2CS in two rotating molecular rings in the HL Tau and IRAS04302+2247 disks. The outer radii are about 140 au (HL Tau), and 115 au (IRAS 04302+2247). The edge-on geometry of IRAS 04302+2247 reveals that H2CS emission peaks, at radii of 60-115 au, at z = +- 50 au from the equatorial plane. The column densities are about 10^14 cm^-2. For HL Tau, we derive, for the first time, the [H2CS]/[H] abundance in a protoplanetary disk (about 10^-14). The BEs of H2CS computed for extended crystalline ice and amorphous ices is 4258 K and 3000-4600 K, respectively, implying a thermal evaporation where dust temperature is larger than 50-80 K. Conclusions: H2CS traces the so-called warm molecular layer, a region previously sampled using CS, and H2CO. Thioformaldehyde peaks closer to the protostar than H2CO and CS, plausibly due to the relatively high-excitation level of observed 7_1,6-6_1,5 line (60 K). The H2CS BEs implies that thermal desorption dominates in thin, au-sized, inner and/or upper disk layers, indicating that the observed H2CS emitting up to radii larger than 100 au is likely injected in the gas due to non-thermal processes.
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Astronomy &Astrophysics manuscript no. Thio ©ESO 2020
November 5, 2020
ALMA chemical survey of disk-outflow sources in Taurus
(ALMA-DOT)
IV. Thioformaldehyde (H2CS) in protoplanetary disks: spatial distributions and
binding energies
C. Codella1,2, L. Podio1, A. Garufi1, J. Perrero3, P. Ugliengo3, D. Fedele1,4, C. Favre2, E. Bianchi2, C. Ceccarelli2, S.
Mercimek1,5, F. Bacciotti1, K.L.J. Rygl6, and L. Testi7,8,1
1INAF, Osservatorio Astrofisico di Arcetri, Largo E. Fermi 5, 50125 Firenze, Italy
2Univ. Grenoble Alpes, CNRS, Institut de Planétologie et d’Astrophysique de Grenoble (IPAG), 38000 Grenoble, France
3Dipartimento di Chimica and Nanostructured Interfaces and Surfaces (NIS) Centre, Università degli Studi di Torino, via P. Giuria
7, 10125 Torino, Italy
4INAF, Osservatorio Astrofisico di Torino, Via Osservatorio 20, I-10025 Pino Torinese, Italy
5Università degli Studi di Firenze, Dipartimento di Fisica e Astronomia, Via G. Sansone 1, 50019 Sesto Fiorentino, Italy
6INAF, Istituto di Radioastronomia & Italian ALMA Regional Centre, via P. Gobetti 101, 40129 Bologna, Italy
7European Southern Observatory, Karl-Schwarzschild-Strasse 2, 85748 Garching bei München, Germany
8Excellence Cluster Origins, Boltzmannstrasse 2, 85748 Garching bei München, Germany
Received date; accepted date
ABSTRACT
Context. Planet formation starts around Sun-like protostars with ages 1 Myr: what is the chemical compositions in disks?
Aims. To trace the radial and vertical spatial distribution of H2CS, a key species of the S-bearing chemistry, in protoplanetary disks. To
analyse the observed distributions in light of the H2CS binding energy, in order to discuss the role of thermal desorption in enriching
the gas disk component.
Methods. In the context of the ALMA chemical survey of Disk-Outflow sources in the Taurus star forming region (ALMA-DOT), we
observed five Class I or early Class II sources with the o–H2CS(71,661,5) line. ALMA-Band 6 was used, reaching spatial resolutions
'40 au, i.e. Solar System spatial scales. We also estimated the binding energy of H2CS using quantum mechanical calculations, for
the first time, for an extended, periodic, crystalline ice.
Results. We imaged H2CS emission in two rotating molecular rings in the HL Tau and IRAS04302+2247 disks. The outer radii are
140 au (HL Tau), and 115 au (IRAS 04302+2247). The edge-on geometry of IRAS 04302+2247 allows us to reveal that H2CS
emission peaks, at radii of 60–115 au, at z=±50 au from the equatorial plane. Assuming LTE conditions, the column densities are
1014 cm2. Upper limits of a few 1013 cm2have been estimated for the H2CS column densities in DG Tau, DG Tau B, and Haro 6-13
disks. For HL Tau, we derive, for the first time, the [H2CS]/[H] abundance in a protoplanetary disk ('1014). The binding energy
of H2CS computed for extended crystalline ice and amorphous ices is 4258 K and 3000-4600 K, respectively, implying a thermal
evaporation where dust temperature is 50–80 K.
Conclusions. H2CS traces the so-called warm molecular layer, a region previously sampled using CS, and H2CO. Thioformaldehyde
peaks closer to the protostar than H2CO and CS, plausibly due to the relatively high-excitation level of observed 71,661,5line (60
K). The H2CS binding energy implies that thermal desorption dominates in thin, au-sized, inner and/or upper disk layers, indicating
that the observed H2CS emitting up to radii larger than 100 au is likely injected in the gas due to non-thermal processes.
Key words. astrochemistry - protoplanetary disks - methods: numerical - ISM: molecules - ISM: individual objects: HL TAU,
IRAS04302+2247
1. Introduction
Low-mass star formation is the process starting from a molecular
cloud and ending with a Sun-like star with its own planetary sys-
tem. According to the classical scenario (e.g. Andre et al. 2000;
Caselli & Ceccarelli 2012, and references therein), the central
object increases its mass through an accretion disk, while a fast
jet contributes in removing the angular momentum excess. While
the star accrete its mass, part of the material in the disk is incor-
porated to form planets. As the physical process proceeds, also
Send oprint requests to: C. Codella, e-mail:
codella@arcetri.astro.it
the chemistry evolves towards a complex gas composition (see
Ceccarelli et al. 2007;Herbst & van Dishoeck 2009). Several ob-
servational programs have been dedicated to the chemical con-
tent of protostellar envelopes/disks using both single-dishes and
interferometers at mm-wavelenghts (IRAM 30-m ASAI (Lefloch
et al. 2018); ALMA PILS (Jørgensen et al. 2016); IRAM PdBI
CALYPSO (Belloche et al. 2020); IRAM NOEMA SOLIS (Cec-
carelli et al. 2017); ALMA FAUST1, Bianchi et al. 2020). Nev-
ertheless, the chemical content of the protoplanetary disks is
still poorly known. Tiny outer molecular layers (and thus small
column densities) are formed due to thermal or UV-photo/CR-
1http://faust-alma.riken.jp
Article number, page 1 of 11
arXiv:2011.02305v1 [astro-ph.EP] 4 Nov 2020
A&A proofs: manuscript no. Thio
induced desorption (e.g., Semenov & Wiebe 2011;Walsh et al.
2014,2016;Loomis et al. 2015;Le Gal et al. 2019). More pre-
cisely, the disk portions where thermal desorption is expected to
rule is in turn determined by the binding energies (BEs) of the
species to grains. Dierent BEs imply dierent temperatures of
the dust which can inject iced molecules into the gas-phase (e.g.,
Penteado et al. 2017).
A recent blooming of projects focused on protoplanetary
disks, mainly with ALMA2, led to the detection of several
molecules from CO isotopologues to complex species such as t-
HCOOH, CH3OH, and CH3CN (see Öberg et al. 2013,2015a,b;
Öberg & Bergin 2016;Guilloteau et al. 2016;Favre et al. 2015,
2018,2019;Fedele et al. 2017;Semenov et al. 2018;Podio et al.
2019,2020a,b;Garufi et al. 2020). The ALMA images allowed
the authors to compare the gas and dust distribution, starting the
first steps of physical-chemical modelling. A breakthrough re-
sult provided by ALMA, through (sub-)mm array observations
of young stellar objects, is that planets start to form already dur-
ing the protostellar phases hence before the classical protoplan-
etary stage with an age of at least 1 Myr. This is indirectely in-
dicated by the presence of rings, gaps, and spirals in disks with
ages less than 1 Myr (see e.g., Sheehan & Eisner 2017;Fedele
et al. 2018;Andrews et al. 2018). These substructures have been
observed also using molecules, driving studies to sample the
molecular components of disks. This is the goal of the ALMA-
DOT project (ALMA chemical survey of Disk-Outflow sources
in Taurus), which targets Class I or early Class II disks to obtain
their chemical characterization.
1.1. The S-bearing molecules
Chemistry of S-bearing species is not well understood. In dense
gas, which is involved in the star forming process, sulphur is
severely depleted (e.g. Wakelam et al. 2004;Phuong et al. 2018;
Tieftrunk et al. 1994;Laas & Caselli 2019;van ’t Hoet al.
2020), by at least two orders of magnitude with respect to the
Solar System value [S]/[H] =1.8 ×105(Anders & Grevesse
1989). The main S-carrier species on dust grains, however, are
still unknown. For years, H2S has been postulated to be the solu-
tion, but so far it has been never directly detected on interstellar
ices (Boogert et al. 2015). Alternative solutions have been pro-
posed in light of studies focused on protostellar shocks, where
dust is sputtered: S, OCS, or H2CS (e.g. Wakelam et al. 2004;
Codella et al. 2005;Podio et al. 2014;Holdship et al. 2016),
but, again, no detection on ices has been reported (Boogert et al.
2015). What about the inventory of S-molecules in protoplan-
etary disks? Only four species have been detected, often by
single-dish: CS, SO, H2S, and H2CS. More specifically, multi-
line CS emission has been observed towards 10 disks (e.g.
Dutrey et al. 1997,2017;Fuente et al. 2010;Guilloteau et al.
2013,2016;Teague et al. 2018;Phuong et al. 2018;Semenov
et al. 2018;Le Gal et al. 2019;Garufi et al. 2020;Podio et al.
2020a). SO emission has been detected in fewer disks, part of
them still associated with accretion, as e.g. TMC-1A (e.g. Fuente
et al. 2010;Guilloteau et al. 2013,2016;Sakai et al. 2016;
Pacheco-Vázquez et al. 2016;Teague et al. 2018;Booth et al.
2018). On the other hand, only very recently H2S and H2CS have
been detected and imaged towards a couple of disks. Namely,
H2S has been imaged towards GG Tau A (Phuong et al. 2018),
while H2CS has been observed with ALMA towards MWC480,
and, tentatively, LkCa 15 (Le Gal et al. 2019;Loomis et al.
2Atacama Large Millimeter Array: https://www.almaobservatory.org
2020). Further observations of the S-species supposed to be the
main S-carrier on dust grains are required.
In this context, the goal of the present project is twofold:
(1) to map the H2CS (thioformaldehyde) spatial distribution in
protoplanetary disks in an intermediate phase between Class I
and Class II, and (2) to derive the binding energies of H2CS us-
ing quantum mechanical calculations for an extended crystalline
ice. We focus on H2CS in the eort to identify S-bearing species
able to trace protoplanetary disks. The article is organized as fol-
lows: we first present the observations and data reduction pro-
cess (Sect. 2), then we report the observational results (Sect. 3),
and present the method and the assumptions used to derive BEs
(Sect. 4). In Sect. 5, the results will be discussed by comparing
the H2CS maps with (i) those of other molecular species as well
as with (ii) the spatial distributions expected in case the ther-
mal desorption process (driven by the BE values) is the main
mechanism leading to H2CS in the gas-phase. Finally, Sect. 6
summarises our work.
2. Observations: sample and data reduction
The sample consists of four Class I and one early Class II (e.g.
Andre et al. 2000) well known sources (Guilloteau et al. 2013,
2014): DG Tau, DG Tau B, HL Tau, IRAS 04302+2247, and
Haro 6–13 (aka V 806 Tau). The sources are observed in the
context of the ALMA-DOT project (ALMA chemical survey of
Disk-Outflow sources in the Taurus star forming region, Podio
et al. 2019,2020a;Garufi et al. 2020), which targets sources: (i)
still embedded in a dense envelope, (ii) driving an atomic jet, and
a molecular outflow. The sources are chemically rich as revealed
by IRAM-30m observations detecting CO isotopologues, H2CO,
and CN (plus SO for all but Haro 6–13) (Guilloteau et al. 2013).
This work is based on ALMA Cycle 4 observations of
DG Tau and DG Tau B and Cycle 6 observations of HL Tau,
IRAS 04302+2247, and Haro 6-13 (projects 2016.1.00846.S and
2018.1.01037.S, PI: L. Podio). The DG Tau and DG Tau B ob-
servations were described by Podio et al. (2019), and Garufi
et al. (2020), respectively. All Band 6 observations were taken
in an extended array configuration with baselines ranging from
15 m to 1.4 km or from 17 m to 3.7 km. The frequency inter-
val covered by the continuum spectral window included the o–
H2CS(71,661,5) line emitting at 244048.5 MHz, characterised3
by Eup =60 K, and Sµ2=56 D2. A standard data reduction was
performed with CASA pipeline version 4.7.2. Self-calibration
was performed on the continuum emission and then applied
to the continuum-subtracted line datacube. The r.m.s. for con-
tinuum images are about 68 µJy (HL Tau) and 40 µJy (IRAS
04302+2247). The line spectral cube was produced through
tclean. We used robust weighting in order to maximise the spa-
tial resolution, and set a channel width of 1.2 km s1. The r.m.s.
per each channel is about 0.8 mJy beam1. The synthesized beam
(HPBW) is 000
.3×000
.3.
3. Observational results
3.1. Continuum and H2CS spatial distributions
Out of the 5 observed targets, we detected o–H2CS(71,6
61,5) emission towards 2 disks, namely HL Tau and IRAS
04302+2247 (herafter IRAS04302). For DG Tau, DG Tau B,
and Haro 6–13 upper limits on H2CS emission will be reported
3The spectral parameters (Maeda et al. 2008) are taken from the
Cologne Database for Molecular Spectroscopy (Müller et al. 2005).
Article number, page 2 of 11
Codella et al.: ALMA-DOT: H2CS in protoplanetary disks
in the next sections. As a reference to analyse molecular emis-
sion, Figure 1 (upper panels) reports the dust continuum emis-
sion. The well known HL Tau disk (d=147 pc; Galli et al. 2018),
with an inclination angle iof 47(e.g ALMA Partnership et al.
2015;Carrasco-González et al. 2019), is well traced, showing a
radius of 150 au. The dust continuum at 227 GHz peaks (118
mJy beam1) at α(J2000) =04h31m38s
.44, δ(J2000) = +18130
5700
.65. On the other hand, the IRAS04302 disk Guilloteau et al.
(2013); Podio et al. (2020a), located at d=161 pc (Galli et al.
2019), is more extended (350 au), and is associated with an
almost edge-on geometry, i90(Wolf et al. 2003). The coor-
dinates of the continuum peak, 133 mJy beam1, are α(J2000) =
04h33m16s
.47, δ(J2000) = +225302000
.36.
Figure 1 (Middle) reports also the intensity integrated maps
(moment 0) of the o–H2CS(71,661,5) emission as observed to-
wards HL Tau and IRAS04302, thus providing for the first time
the thioformaldeyde radial (HL Tau) and vertical (IRAS04302)
distributions. All the channels showing emission of at least 3σ
(see Sect. 2) have been used, namely: 3–11 km s1(HL Tau) and
2–10 km s1(IRAS04302). The Signal-to-Noise (S/N) of the ve-
locity integrated emission is, in both sources, larger than 8. For
HL Tau, the image clearly shows an H2CS ring around a central
dip. The outer radius is about 140 pc, while the dip is confined
in the inner 35 au. For IRAS04302, the picture as provided
by the mom 0 map is less clear. Surely, the H2CS emission is
confined in the inner 000
.7, 115 au. In Sect. 3, we will show
how kinematics will lead us to infer the structure of the emitting
region.
Finally, Figure 1 (Bottom panels) reports, in colour scale, the
HL Tau and IRAS04302 H2CS(71,661,5) spatial distributions
of the peak intensity as derived using the moment 8 method4to
enlight the images. The moment 8 CASA algorithm has been
used by collapsing the intensity axis of the ALMA datacube to
one pixel and setting the value of that pixel (for R.A. and Dec.)
to the maximum value of the spectrum. The moment 8 images
definitely confirm what found with the moment 0 maps. In Sect.
5.2, the spatial distribution will be compared with those of other
molecular species.
3.2. H2CS kinematics
Figures 2 and 3 summarise the kinematics of HL Tau and
IRAS04302 provided by: (i) channel maps, (ii) intensity
weighted mean velocity (moment 1) maps, and (iii) H2CS spec-
tra as extracted towards the brightest positions. The H2CS in HL
Tau is clearly rotating with the blue- and red-shifted sides lo-
cated towards SE and NW, respectively. The systemic velocity
is +7.0 km s1(in agreement with ALMA Partnership et al.
2015;Wu et al. 2018). The same rotating gradient has been ob-
served using HCO+(ALMA Partnership et al. 2015;Yen et al.
2019), C18O (Wu et al. 2018), and 13C17 O (Booth & Ilee 2020).
Also the emission towards IRAS04302 disk shows a rotation pat-
tern. Its almost edge-on orientation allows us to clearly disen-
tangle the red- (southern) and blue-shifted (northern) lobes. The
systemic velocity estimated from the velocity distribution of the
bright H2CO line is +5.6 km s1(Podio et al. 2020a), in good
agreement with IRAM 30-m CN, H2CO, CS, and C17O spec-
tra of Guilloteau et al. (2013,2016). The rotation pattern has
been imaged also by Podio et al. (2020a), who found, using CO,
H2CO, and CS emission, a molecular emission which is verti-
cally stratified (see Sect. 4 for the comparison with H2CS).
4https://casa.nrao.edu/Release3.4.0/docs/UserMan/UserManse41.html
The H2CS channel maps show that the emission shifted by
less than 2 km s1is emitted from the inner 000
.5 region, whereas
at larger velocities we detect emission up to 100
.2 from the proto-
star. This suggests that larger projected velocities (in particular
the blue-shifted velocity) have a larger projected positional oset
from the protostar. In other words, the present dataset suggests
that V R. This is the standard signature of a rotating ring with
an inner dip, and not a filled disk, where we would have an oppo-
site trend, with V R2. Very recently, Oya & Yamamoto (2020)
reported the detection of H2CS in the IRAS16293 A protostellar
disk (see also van ’t Hoet al. 2020). In addition, the present
findings well resamble what found in the archetypical protostel-
lar disk HH212, also close to be edge-on as IRAS04302 (e.g. Lee
et al. 2019, and references therein). Also in this case, a chemi-
cal enrichment in the gas phase associated with rotating rings is
revealed by the V R kinematical feature (see e.g. the recent
review by Codella et al. 2019).
3.3. H2CS column densities and abundances
Assuming (i) Local Thermodynamic Equilibrium (LTE), and (ii)
optically thin emission, the column densities of the H2CS are de-
rived. The first assumption is well justified as the H2gas density
in the molecular layers is larger than 107cm3(see e.g. Walsh
et al. 2014;Le Gal et al. 2019), i.e. well above the critical density
of the considered o-H2CS(71,6–61,5) line (ncr a few 104cm3in
the 20–150 K range5. The second assumption is justified as mod-
els indicate an abundance (with respect to H) of H2CS lower than
1010 (Le Gal et al. 2019;Loomis et al. 2020).
In HL Tau the observed emitting area is 1.35 arcsec2(from
the moment 0 map) the flux is 148 mJy km s1(2.6 K km s1). Le
Gal et al. (2019) estimated an H2CS rotational temperature be-
tween 20 K and 80 K in the MWC 480 disk. We conservatively
adopted a temperature between 20 K and 150 K. An ortho-to-
para ratio of 3, i.e. the statistical value, has been assumed (as
done by Le Gal et al. 2019). The total H2CS column density (av-
eraged on the emitting area) NH2CS turns out to be 0.9–1.4 ×1014
cm2. For IRAS04302 the emitting area is smaller with respect
to HL Tau, 0.72 arcsec2and the flux is '78 mJy km s1(2.5
K km s1). The column density NH2CS is, similarly to HL Tau, '
1014 cm2. These values can be also considered as an a-posteriori
check that the observed H2CS emission is optically thin. Indeed,
by assuming kinetic temperatures larger than 20 K and densi-
ties larger than 107cm3, the Large Velocity Gradient approach
confirms that column densities around 1014 cm2implies for the
o-H2CS(71,6–61,5) line an opacity of 0.1. These column density
estimates are larger by a factor 30 with respect to the ones mea-
sured by Le Gal et al. (2019) and Loomis et al. (2020) towards
the massive disk MWC 480 (3 ×1012 cm2). However, as re-
ported by the authors, their spatial resolution is not high enough
to evaluate the presence of a central dip, which could cause an
underestimate the H2CS column density.
For HL Tau a further step can be done given that Booth &
Ilee (2020) published an ALMA map of the 13C17 O(3–2) emis-
sion at a similar angular scale as our H2CS maps. The 13C17O
spatial distributions well agrees with that of H2CS. The emis-
sion is considered optically thin, given that its abundance ratio
with respect to 12C16 O is 8.3 ×106(Milam et al. 2005). Tak-
ing the 13C17 O flux density of 10-20 mJy beam1km s1, and an
excitation temperature, as for H2CS, in the 20-150 K range, we
derive NCO '5–10 ×1023 cm2. Using [CO]/[H] =5×105, the
5Using scaled H2CO collisional rates from Wiesenfeld & Faure
(2013), see Schöier et al. (2005).
Article number, page 3 of 11
A&A proofs: manuscript no. Thio
H2CS abundance (with respect to H) results to be X(H2CS )'
1014. The comparison with the H2CS abundances predicted by
disk chemistry is challenging, given this is dramatically depend-
ing on the initial composition of the S-species, which can vary by
orders of magnitude (see e.g Fedele & Favre 2020). Vice versa,
the present measured H2CS abundances will be hopefully used
in future chemical models to constrain their initial conditions.
Finally, the upper limits on the H2CS column densities in
DG Tau, DG Tau B, and Haro 6-13, derived taking the 5σlevel
of the moment 0 maps, and using all the assumptions as above,
are: NH2CS 2×1013 cm2(DG Tau B), and NH2CS 4×1013
cm2(DG Tau and Haro 6-13).
4. Binding energies: ice modelling and
computational methods
We computed the H2CS and CS BEs, adopting for the bulk ice
a proton-ordered (P-ice) crystalline model (Casassa et al. 1997).
The ice surface where the adsorption takes place was simulated
by a finite slab model of the (010) surface cut out from the bulk
P-ice crystal, as recently proposed by Ferrero et al. (2020) to pre-
dict the BEs of a set of 21 molecules using the periodic ab initio
program CRYSTAL17 (Dovesi et al. 2018). CRYSTAL17 adopts
localised (Gaussian) basis functions which allow to simulate the
surfaces as a true 2D systems, without including fake replicas of
the slab separated by artificial voids. The surface slab model is
thick enough (number of water layers) to ensure a converged sur-
face energy (energy penalty to cut the surface from the bulk ice).
The choice of a crystalline ice model is against the overwhelm-
ing evidence that ice in the interstellar environment is of amor-
phous nature (AWS). There are two main reasons that hinder the
adoption of AWS phase at the modeling level: i) the experimen-
tal atomistic structure of the AWS is unknown; ii) AWS model
should be based on very large unit cell to mimic the disorder na-
ture of the ice. Point i) means that the model cannot be derived
from experimental evidence and therefore any model is some-
how arbitrary. Point ii) implies that very expensive calculations
are needed to cope with the large unit cells. In the following, we
proposed a simplified strategy to derive the values of the BEs
for the H2CS and CS molecules as adsorbed on AWS, without
actually run the needed expensive calculations, but taking profit
of the results by Ferrero et al. (2020) on the analogous CO and
H2CO molecules, in which both crystalline and AWS models
were studied.
First, we set up the starting locations of H2CS and CS
molecules at the ice surface using the optimized positions of the
analogous CO and H2CO molecules after Ferrero et al. (2020)
and then fully optimizing the structures. We choose the HF-3c
method, which combines the Hartree-Fock Hamiltonian with the
minimal basis set MINI-1 (Tatewaki & Huzinaga 1980) sup-
plemented by three a posteriori corrections for: (i) the basis
set superposition error (BSSE), arising when localized Gaussian
functions are used to expand the basis set (Jansen & Ros 1969;
Liu & McLean 1973); (ii) the dispersive interactions; (iii) short-
ranged deficiencies due to the adopted minimal basis set (Sure &
Grimme 2013). The resulting optimized unit cell of the ice (010)
surface is shown in Figure 4, together with the mapping of the
electrostatic potential (ESP) computed at HF-3c level of theory.
The ESP reveals the oxygen rich (red color, ESP <0) and pro-
ton rich (blue color, ESP >0) regions, acting, respectively, as a
H-bond acceptor/donor with respect to specific adsorbates.
In order to get accurate BEs, the HF-3c structures were used
to compute single point energy evaluation at B3LYP-D3(BJ)
level of theory (Becke 1993). Dispersion interaction is included
through the D3 correction, with the Becke-Johnson damping
scheme (Grimme et al. 2010). The Ahlrichs’ triple-zeta qual-
ity VTZ basis set, supplemented with a double set of polariza-
tion functions (Schäfer et al. 1992) was adopted to define the fi-
nal B3LYP-D3(BJ)/A-VTZ*//HF-3c model chemistry. BEs were
also corrected for BSSE.
For H2CS, the most stable structure shows a symmetric in-
volvement of the CH2S molecule with the ice surface, in which
the C-H bonds act as weak H-donors toward the surface oxygen
atoms, while the S atom as a H-bond acceptor at the dangling
surface OH groups. For CS, the adsorption occurs through the
C-end with a very long H-bond with the dangling ice OH group.
Any attempt to engage the CS molecule through the S end of the
molecule evolved spontaneously to the C-end one. Obviously,
the relatively simple structure of the crystalline P-ice does not
allow to explore other configurations than the described ones,
at variance with the results for an AWS model which would be
expected to provide a many-fold of adsorption sites of dierent
strength. Furthermore, due to the long range order of the water
molecules in the crystalline ice, the H-bond interactions will co-
operate to enhance the H-bond donor/acceptor character of the
surface water molecules, giving very high/low values of the ESP
(see Figure 4). This means that the BEs resulting from the crys-
talline model should be taken as an upper limit, as shown by
Ferrero et al. (2020). As anticipated, to remedy the deficiencies
of the crystalline ice model we resort to data from the work by
Ferrero et al. (2020) for the analog CO and H2CO molecules
(with respect to CS and H2CS treated here) adsorbed on the
AWS model. As expected, they found a rather complex adsorp-
tion scenario at AWS, when compared to that occurring at the
P-ice surface. For CO, five dierent adsorption sites have been
characterized; for H2CO, up to eight dierent adsorption sites
were predicted. Obviously, each of these adsorption sites pro-
vides dierent values of the BE and in the limit of very large
AWS models, the BE values will obey to a certain distribution.
It is clear that a similar painstacking study should be carried out
also for CS and H2CS. Instead, as anticipated, we resort to a
simplified scheme to guess the BE values for the AWS, without
actually running any calculation.
First, from the data by Ferrero et al. (2020), we worked out
two scaling factors (0.859 and 0.775, respectively) connecting
the BE of the CO and H2CO analogs computed for the P-ice
to their corresponding averaged BE values for the AWS model.
Then by assuming the same scaling factors also for the present
CS and H2CS cases, we scaled the BEs for the crystalline ice
to estimate their averaged values on the AWS model. In agree-
ment with the CO and H2CO cases, also for CS and H2CS the
BE-AWS are smaller than those for the crystalline ice. Table 1
reports, for both H2CS and CS, the derived BEs on crystalline
(H2CS: 4258 K; CS: 3861 K) and AWS (H2CS: 3000-4600 K;
CS: 2700-4000 K) ice.
5. Discussion
5.1. Comparison with previous BEs measurements
Interstellar molecules are formed either through gas-phase re-
actions or directly on grain surfaces. Regardless of the forma-
tion route, gaseous molecules freeze out into the grain mantles
in timescales that depend on the density and temperature of the
gas and dust as well as the molecule BE. Thus, in cold and dense
regions, as in the outer disk regions and in the layers close to the
disk midplane, icy mantles envelope the dust grains. The frozen
Article number, page 4 of 11
Codella et al.: ALMA-DOT: H2CS in protoplanetary disks
Table 1. H2CS and CS BEs (Kelvin) derived for the crystalline (CRY)
and amorphous (AWS) ice models. See the text for the procedure
adopted to arrive to the BE-AWS values
BE-CRY BE-AWS DasaWakelamb
H2CS 4258 3000–4600 3110 4400
CS 3861 2700–4000 2217 3200
aDas et al. (2018); bWakelam et al. (2017).
molecules can then be injected into the gas-phase via three pro-
cesses (see e.g. Walsh et al. 2014): (i) thermal desorption, (ii)
UV-photo and/or CR-induced desorption, and (iii) reactive des-
orption. The first process occurs inside the so called snow lines,
i.e. the location where the dust temperature is high enough to
allow the species to sublimate.
Regarding H2CO, its BE has been experimentally measured
on amorphous water surface (AWS) through thermal desorption
process, e.g. by Noble et al. (2012) to be 3260±60 K, and esti-
mated via theoretical computations on AWS and crystalline ice
models by Ferrero et al. (2020), who found zero point corrected
BEs (see Sect. 4) in the 3071-6194 K range, for the AWS case,
therefore bracketing the experimental value. The BE for the crys-
talline ice falls at 5187 K, in the higher regime of the AWS range.
Following the described procedure, we found for H2CS BE
values of 4258 K and 3000–4600 K for the crystalline and AWS
ice models, respectively. For CS, we have slightly lower values:
3861 K (crystalline) and 2700–4000 K (AWS). Table 1compares
our results with the available literature data, all coming from
computer simulations. The BE computed by Das et al. (2018),
who adopted a tetramer of water molecules to simulate the ice,
are in the low end of our computed BEs range, whereas the BE
computed by Wakelam et al. (2017), based on one single water
and corrected with an empirical factor, lies on the high end of
our range.
Based on our new computations of Sect. 4 and using a BE
ranging from 3000 to 4600 K, H2CS is expected to thermally
sublimate in regions of the disk where the dust temperature ex-
ceeds 50 to 80 K, respectively. We emphasise that the disper-
sion in our computed BEs reflects the dierent possible sites of
adsorption of H2CS and it is, therefore, physical and not due to
a computational uncertainty (see the discussion in Ferrero et al.
2020). Although we cannot a priori say how many sites with
each dierent BE are populated, we can conservatively assume
that H2CS molecules should remain frozen in regions of the disk
with dust temperatures lower than 50–80 K. The fact that H2CS
emission up to outer radii of 140 au (HL Tau) and 115 au
(IRAS 04302) suggests that non thermal processes are likely re-
sponsible for the presence of H2CS in the gas in those disk re-
gions.
5.2. Comparison between H2CS, CS, and H2CO
The formation routes of H2CS have been recently summarised
by Le Gal et al. (2019), who used the the gas-grain chem-
ical model Nautilus (Wakelam et al. 2016) supported by the
gas chemical dataset KIDA (Wakelam et al. 2015), and by
Fedele & Favre (2020), who adopted the thermo-chemical model
DALI (Bruderer et al. 2012), coupled with the chemical network
UMIST (Woodall et al. 2007). Generally, H2CS is mainly (99%)
formed in gas-phase via neutral–neutral reaction of atomic S
with CH3. On the other hand, CS in disks is also thought to
be mainly formed in gas-phase, through reactions starting with
small hydrocarbons interacting with S+(in upper disk layers) or
S (in inner slabs). Finally, H2CO can be formed on grains due
to hydrogenation processes as well and in gas-phase by oxygen
reacting with CH3, in a analogous way of S +CH3H2CS (see
e.g. Fedele & Favre 2020, and references therein).
For the IRAS04302 disk, the H2CS vertical intensity profile
can be compared with those of CS and formaldehyde (H2CO),
by Podio et al. (2020a). For such a purpose, we averaged the
emission radially over 3 pixels (000
.18, corresponding to 29 au)
around the selected radius. Figure 5reports the comparison ob-
tained at 60 au and 115 au from the protostar. Note that the H2CS
intensity has been multiplied by the factor reported in the labels
in order to better compare with those of o-H2CO and CS. The
vertical distribution of H2CS (black) shows an asymmetry with
respect to the disk midplane (i.e. z=0), with the emission from
the eastern disk side being brighter than in the western side by
a factor 1.8 at 60 au radial distance and a factor 1.5 at 115 au.
The same asymmetry in the vertical distribution is observed in
the H2CO (blue) and CS (red) emission, and all the three species
peak at a disk height, zof about 50 au. This suggests that at
our resolution the emission from H2CS, H2CO, and CS orig-
inate from the same disk layer. As discussed by Podio et al.
2020, the bulk of the H2CO and CS emission originate from the
disk molecular layer where molecules are either released from
dust grains and/or formed in gas-phase. Given that H2CS is co-
spatial with H2CO and CS and that all the three molecules can be
eciently formed in gas-phase using small hydrocarbons (e.g.
CH3), we suggest that H2CS may form in similar way.
The comparison between the moment 0 distributions of
H2CS with those of H2CO (Podio et al. 2020a) is also instruc-
tive (see Fig. 6), showing a slightly dierent radial distribution
of H2CO and H2CS. The H2CO (and CS) emissions extend ra-
dially out to 480 au and peak at 120 au, while the H2CS
emission is radially confined in the inner 115 au with a peak at
70 au. The radial distribution of H2CS suggests that the o–
H2CS(71,6–61,5) line probes an inner portion of the IRAS04302
disk, possibly due a higher Eup, 60 K, with respect to those of
the o–H2CO(31,2–21,1) and CS(5–4), 33–35 K. Only further ob-
servations of a species using dierent excitation lines will shed
light on this hypothesis.
6. Conclusions
We presented the first images of the radial (HL Tau) and verti-
cal (IRAS04302) spatial distribution of the o-H2CS emission as
observed towards Class I protoplanetary disks using ALMA on
a Solar System scale. The observations have been performed in
in the context of the ALMA chemical survey of Disk-Outflow
sources in the Taurus star forming region (ALMA-DOT). H2CS
is confined in a rotating ring with an inner dip towards the
protostar: the outer radii are 140 au (HL Tau) and 115 au
(IRAS04302). The edge-on geometry of IRAS 04302 allows us
to reveal that H2CS emission peaks, (at r=60–115 au), at z=
±50 au from the equatorial plane. Assuming LTE conditions,
the column densities are 1014 cm2. For HL Tau, we derived,
for the first time, the [H2CS]/[H] abundance in a protoplanetary
disk ('1014). The o–H2CS(71,661,5) line emits where the emis-
sion of CS(5–4) and o–H2CO(31,221,1) is brighter (Podio et al.
2020a), i.e. the so-called warm molecular layer. H2CS emission
peaks closer to the protostar with respect to H2CO and CS, pos-
sibly due to the higher energy of the upper level (60 K) of the
observed transition with respect to those of H2CO and CS (33-
35 K), which requires higher gas temperature hence favouring
the emission from the inner disk regions.
Article number, page 5 of 11
A&A proofs: manuscript no. Thio
The present work also provides the H2CS and CS BEs as
computed for the first time for an extended crystalline ice (4258
K, H2CS, and 3861 K, CS) and estimated for an AWS model
using recipes from previous work (Ferrero et al. 2020) to be in
the 3000-4600 K and 2700-4000 K range. In turn, for 1L
protostars, this implies that radially thermal desorption rules in
an inner region, while vertically only a thin upper layer is hot
enough (see e.g. Walsh et al. 2014;Le Gal et al. 2019). To con-
clude, the observed H2CS, more precisely that detected at radii
up to more than 100 au, is released into the gas likely due to
non-thermal processes (photo-/CR- and/or reactive-desorption).
Acknowledgements. We thank the anonymous referee for instructive discussion
and suggestions. This paper uses the ADS/JAO.ALMA 2016.1.00846.S and
ADS/JAO.ALMA 2018.1.01037.S (PI L. Podio) ALMA data. ALMA is a part-
nership of ESO (representing its member states), NSF (USA) and NINS (Japan),
together with NRC (Canada), MOST and ASIAA (Taiwan), and KASI (Republic
of Korea), in cooperation with the Republic of Chile. This work was supported
by the European Research Council (ERC) under the European Union’s Horizon
2020 research and innovation programmes: (i) "The Dawn of Organic Chem-
istry" (DOC), grant agreement No 741002, and (ii) “Astro-Chemistry Origins”
(ACO), Grant No 811312. CF acknowledges financial support from the French
National Research Agency in the framework of the Investissements d’Avenir pro-
gram (ANR-15-IDEX-02), through the funding of the "Origin of Life" project of
the Univ. Grenoble-Alpes. DF acknowledges financial support from the Italian
Ministry of Education, Universities and Research, project SIR (RBSI14ZRHR).
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Article number, page 6 of 11
Codella et al.: ALMA-DOT: H2CS in protoplanetary disks
Fig. 1. Upper panels: Map (cyan contours and colour scale) of the 1.3mm dust continuum distribution for HL Tau (Left) and IRAS 04302+2247
(Right) disks. First contours and steps are 3σ(200 µJy beam1, HL Tau; 115 µJy beam1, IRAS 04302+2247), and 200σ, respectively. The ellipse
in the bottom left corner shows the ALMA synthesized beam (HPBW): 000
.28 ×000
.25 (PA =–7), for HL Tau, and 000
.28 ×000
.22 (PA =–3), for
IRAS 04302+2247. Middle panels: Spatial distribution (moment 0) maps (white contours and colour scale) of the o–H2CS(71,6–61,5) line based
on the velocity integrated emission (3–11 km s1, HL Tau, 2–10 km s1, IRAS 04302+2247), overlaid on the continuum maps (cyan contours).
First contours and steps are 5σ(7.5 mJy beam1km s1, HL Tau, and 12.5 mJy beam1km s1, IRAS04302), and 3σ, respectively. The ellipse
shows the synthesized beam (HPBW): 000
.29 ×000
.27 (PA =2), for HL Tau, and 000
.30 ×000
.26 (PA =2), for IRAS 04302+2247. Lower panels:
Moment 8 maps (white contours and colour scale) of the H2CS(71,6–61,5) based on the same velocity integrated emission used for the moment 0
maps, overlaid on the continuum maps (cyan contours). First contours and steps are 5σ(3 mJy beam1km s1), and 3σ, respectively.
Article number, page 7 of 11
A&A proofs: manuscript no. Thio
Fig. 2. Upper: Channel maps of the o–H2CS(71,6–61,5) blue- and red-shifted emission in the HL Tau disk. Each panel shows the emission
integrated over a velocity interval of 1.2 km s1shifted with respect to the systemic velocity (+7 km s1, green) by the value given in the
upper-right corner. We report, in black, the 3σcontour of the continuum emission (Figs. 1, A.1). The black triangles indicate where spectra have
been extracted. The ellipse shows the synthesized beam (HPBW): 000
.29 ×000
.27 (PA =2). First contours and steps correspond to 3σ(2.1 mJy
beam1) and 1σ, respectively. Osets are derived with respect to the continuum peak (Sect. A). Bottom Left: o–H2CS(71,6–61,5) spectra in flux
and brightness temperature scales (Tb/Fν=328.593) extracted in the positions marked with a red or blue triangle in the Upper panels. Bottom
Right: First-moment map in colour scale.
Article number, page 8 of 11
Codella et al.: ALMA-DOT: H2CS in protoplanetary disks
Fig. 3. Upper: Channel maps of the o–H2CS(71,6–61,5) blue- and red-shifted emission in the IRAS 04302+2247 disk. Each panel shows the
emission integrated over a velocity interval of 1.2 km s1shifted with respect to the systemic velocity (+5.6 km s1Podio et al. 2020a, green) by
the value given in the upper-right corner. We report,in black, the 3σcontour of the continuum emission (Figs. 1, A.1). The black triangles indicate
where spectra have been extracted. The ellipse shows the synthesized beam (HPBW): 000
.30 ×000
.26 (PA =2). First contours and steps correspond
to 3σ(2.1 mJy beam1) and 1σ, respectively. Osets are derived with respect to the continuum peak (Sect. A). Bottom Left: o–H2CS(71,6–61,5)
spectra in flux and brightness temperature scales (Tb/Fν=328.593) extracted in the positions marked with a red or blue triangle in the Upper
panels. Bottom Right: First-moment map in colour scale.
Article number, page 9 of 11
A&A proofs: manuscript no. Thio
Fig. 4. HF-3c optimized P-ice slab model. The adsorption crystallo-
graphic plane is the Miller (010) one. A Panel: Side view along the b
lattice vector. B Panel: Top view of the 2 ×1 supercell (|a|=9.065 Å
and |b|=7.154 Å) along with its ESP map. Colour code: +0.02 atomic
unit (blue, positive), 0.00 atomic unit (green, neutral) and –0.02 atomic
unit (red, negative).
Fig. 5. Vertical intensity profile zof H2CS (black) compared with those
of CS(5–4) (red) and o-H2CO(31,221,1) (blue), from Podio et al.
(2020a). Only fluxes above 3σconfidence are shown. The H2CS in-
tensity has been scaled in order to better compare its profile with those
of o-H2CO and CS. The inner 100
.8 region is shown, with the positive
(negative) values sampling the eastern (western) side. The angular res-
olution is 000
.25 (40 au). The profiles obtained at 60 au (Upper panel)
and 115 au (Lower panel) from the protostar.
Article number, page 10 of 11
Codella et al.: ALMA-DOT: H2CS in protoplanetary disks
Fig. 6. Spatial distribution (moment 0) maps (white contours) of the
o–H2CS(71,6–61,5) line (see Fig. 1), overlaid on the o-H2CO(31,221,1)
reported by Podio et al. (2020a), in black contours and red scale. Sym-
bols are as in Figure 1.
Article number, page 11 of 11
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The method of dispersion correction as an add-on to standard Kohn-Sham density functional theory (DFT-D) has been refined regarding higher accuracy, broader range of applicability, and less empiricism. The main new ingredients are atom-pairwise specific dispersion coefficients and cutoff radii that are both computed from first principles. The coefficients for new eighth-order dispersion terms are computed using established recursion relations. System (geometry) dependent information is used for the first time in a DFT-D type approach by employing the new concept of fractional coordination numbers (CN). They are used to interpolate between dispersion coefficients of atoms in different chemical environments. The method only requires adjustment of two global parameters for each density functional, is asymptotically exact for a gas of weakly interacting neutral atoms, and easily allows the computation of atomic forces. Three-body nonadditivity terms are considered. The method has been assessed on standard benchmark sets for inter- and intramolecular noncovalent interactions with a particular emphasis on a consistent description of light and heavy element systems. The mean absolute deviations for the S22 benchmark set of noncovalent interactions for 11 standard density functionals decrease by 15%-40% compared to the previous (already accurate) DFT-D version. Spectacular improvements are found for a tripeptide-folding model and all tested metallic systems. The rectification of the long-range behavior and the use of more accurate C(6) coefficients also lead to a much better description of large (infinite) systems as shown for graphene sheets and the adsorption of benzene on an Ag(111) surface. For graphene it is found that the inclusion of three-body terms substantially (by about 10%) weakens the interlayer binding. We propose the revised DFT-D method as a general tool for the computation of the dispersion energy in molecules and solids of any kind with DFT and related (low-cost) electronic structure methods for large systems.
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A periodic Hartree-Fock ab initio study is presented concerning two proton-ordered structures of ordinary ice: one ferro-electric (C-ice), the other anti-ferro-electric (P-ice). The calculated energies are practically coincident, and in good agrement with the experimental stability of disordered ice Ih. Slabs are cut out from these crystals in order to formulate a model for studying the surface properties of ordinary ice. The stability of these two-dimensional periodic systems is discussed, and the relaxation of the P-ice slab formed by two bilayers parallel to the (001) face is considered. Finally, an embedded cluster method is adopted to calculate geometric and energetic properties of KOH and NaOH dissolved in C- and P-ice at low concentration. This study permits us to discuss the role of KOH in promoting the transition from disordered Ih to ordered C-ice, which has been observed to occur at 72 K [Leadbetter &etal;, J. Chem. Phys. 82, 424 (1985)].
Article
Non-empirical calculations with Gaussian functions have been performed for several configurations of protonated carbon monoxide.The stablest configuration of protonated CO appears to be a linear [HCO]+ structure. The CO distance in this structure is 0.02 Å smaller than in CO itself and the energy of the system is 152 kcal/mole below the CO-energy.
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