Homogeneous Ice Nucleation Research Articles

Modeling homogeneous ice nucleation from drop-freezing experiments: impact of droplet volume dispersion and cooling rates

Modeling homogeneous ice nucleation from drop-freezing experiments: impact of droplet volume dispersion and cooling rates

Bridging classical nucleation theory and molecular dynamics simulation for homogeneous ice nucleation.

Water freezing, initiated by ice nucleation, occurs widely in nature, ranging from cellular to global phenomena. Ice nucleation has been experimentally proven to require the formation of a critical ice nucleus, consistent with classical nucleation theory (CNT). However, the accuracy of CNT quantitative predictions of critical cluster sizes and nucleation rates has never been verified experimentally. In this study, we circumvent this difficulty by using molecular dynamics (MD) simulation. The physical properties of water/ice for CNT predictions, including density, chemical potential difference, and diffusion coefficient, are independently obtained using MD simulation, whereas the calculation of interfacial free energy is based on thermodynamic assumptions of CNT, including capillarity approximation among others. The CNT predictions are compared to the MD evaluations of brute-force simulations and forward flux sampling methods. We find that the CNT and MD predicted critical cluster sizes are consistent, and the CNT predicted nucleation rates are higher than the MD predicted values within three orders of magnitude. We also find that the ice crystallized from supercooled water is stacking-disordered ice with a stacking of cubic and hexagonal ices in four representative types of stacking. The prediction discrepancies in nucleation rate mainly arise from the stacking-disordered ice structure, the asphericity of ice cluster, the uncertainty of ice-water interfacial free energy, and the kinetic attachment rate. Our study establishes a relation between CNT and MD to predict homogeneous ice nucleation.

The effects of warm-air intrusions in the high Arctic on cirrus clouds

Abstract. Warm-air intrusions (WAIs) are responsible for the transportation of warm and moist air masses from the mid-latitudes into the high Arctic (> 70° N). In this work, we study cirrus clouds that form during WAI events (WAI cirrus) and during undisturbed Arctic conditions (AC cirrus) and investigate possible differences between the two cloud types based on their macrophysical and optical properties with a focus on relative humidity over ice (RHi). We use airborne measurements from the combined high-spectral-resolution and differential-absorption lidar, WALES, performed during the HALO-(AC)3 campaign. We classify each research flight and the measured clouds as either AC or WAI, based on the ambient conditions, and study the macrophysical, geometrical and optical characteristics for each cirrus group. As our main parameter we choose the relative humidity over ice (RHi), which we calculate RHi by combining the lidar water vapor measurements with model temperatures. Ice formation occurs at certain RHi values depending on the dominant nucleation process taking place. RHi can thus be used as an indication of the nucleation process and the structure of cirrus clouds. We find that during WAI events the Arctic is warmer and moister and WAI cirrus clouds are both geometrically and optically thicker compared to AC cirrus. WAI cirrus clouds and the layer directly surrounding them are more frequently supersaturated, also at high supersaturations over the threshold for homogeneous ice nucleation (HOM). AC cirrus clouds have a supersaturation-dominated cloud top and a subsaturated cloud base. WAI cirrus clouds also have high supersaturations at cloud top but also at cloud base.

Phase and Morphology of Water-ice Grains Formed in a Cryogenic Laboratory Plasma

Grains of ice are formed spontaneously when water vapor is injected into a weakly ionized laboratory plasma in which the background gas has been cooled to cryogenic temperatures comparable to those of deep space. These ice grains are levitated indefinitely within the plasma so that their time evolution can be observed under free-floating conditions. Using microscope imaging, ice grains are shown to have a spindle-like fractal structure and grow over time. Both crystalline and amorphous phases of ice are observed using Fourier transform infrared spectroscopy. A mix of crystalline and amorphous grains coexists under certain thermal conditions, and a linear mixing model is used on the ice absorption band surrounding 3.2 μm to examine the ice phase composition and its temporal stability. The extinction spectrum is also affected by inelastic scattering as grains grow, and characteristic grain radii are obtained from Mie scattering theory and compared to size measurements from direct imaging. Observations are used to compare possible ice nucleation mechanisms, and it is concluded that nucleation is likely catalyzed by ions, as ice does not nucleate in the absence of plasma and impurities are not detected. Ice grain properties and infrared extinction spectra show similarity to observations of some astrophysical ices observed in protoplanetary disks, implying that the fractal morphology of the ice and observed processes of homogeneous ice nucleation could occur as well in such astrophysical environments with weakly ionized conditions.

An entropic theory of homogeneous ice nucleation in non-ionic aqueous solutions.

The nucleation of ice from aqueous solutions is a process essential to myriad environmental and industrial processes, but the physical factors affecting the capacity of different solutes to depress the homogeneous nucleation temperature of ice are yet poorly understood. In this work, we demonstrate that for many binary aqueous solutions of non-ionic solutes, this depression is dominated by the entropy of the liquid phase. Employing the classic Turnbull interpretation of the interfacial free energy γ∼TSliquid-Ssolid and estimating solution entropies with a Flory-style modification of the ideal entropy of mixing that accounts for solute size effects, we demonstrate that mixing entropy alone predicts experimental homogeneous nucleation temperatures across a wide variety of non-ionic solutions. We anticipate that this physical insight will not only enhance a fundamental understanding of homogeneous nucleation processes across fields but also open new avenues to the rational design of aqueous solutions for desired nucleation behaviors.

The limit of macroscopic homogeneous ice nucleation at the nanoscale.

Nucleation in small volumes of water has garnered renewed interest due to the relevance of pore condensation and freezing under conditions of low partial pressures of water, such as in the upper troposphere. Molecular simulations can in principle provide insight on this process at the molecular scale that is challenging to achieve experimentally. However, there are discrepancies in the literature as to whether the rate in confined systems is enhanced or suppressed relative to bulk water at the same temperature and pressure. In this study, we investigate the extent to which the size of the critical nucleus and the rate at which it grows in thin films of water are affected by the thickness of the film. Our results suggest that nucleation remains bulk-like in films that are barely large enough accommodate a critical nucleus. This conclusion seems robust to the presence of physical confining boundaries. We also discuss the difficulties in unambiguously determining homogeneous nucleation rates in nanoscale systems, owing to the challenges in defining the volume. Our results suggest any impact on a film's thickness on the rate is largely inconsequential for present day experiments.

Freeze-Induced Phase Transition and Local Pressure in a Phospholipid/Water System: Novel Insights Were Obtained from a Time/Temperature Resolved Synchrotron X-ray Diffraction Study.

Water-to-ice transformation results in a 10% increase in volume, which can have a significant impact on biopharmaceuticals during freeze-thaw cycles due to the mechanical stresses imparted by the growing ice crystals. Whether these stresses would contribute to the destabilization of biopharmaceuticals depends on both the magnitude of the stress and sensitivity of a particular system to pressure and sheer stresses. To address the gap of the "magnitude" question, a phospholipid, 1,2-dipalmitoyl-sn-glycero-3-phosphocholine (DPPC), is evaluated as a probe to detect and quantify the freeze-induced pressure. DPPC can form several phases under elevated pressure, and therefore, the detection of a high-pressure DPPC phase during freezing would be indicative of a freeze-induced pressure increase. In this study, the phase behavior of DPPC/water suspensions, which also contain the ice nucleation agent silver iodide, is monitored by synchrotron small/wide-angle X-ray scattering during the freeze-thaw transition. Cooling the suspensions leads to heterogeneous ice nucleation at approximately -7 °C, followed by a phase transition of DPPC between -11 and -40 °C. In this temperature range, the initial gel phase of DPPC, Lβ', gradually converts to a second phase, tentatively identified as a high-pressure Gel III phase. The Lβ'-to-Gel III phase transition continues during an isothermal hold at -40 °C; a second (homogeneous) ice nucleation event of water confined in the interlamellar space is detected by differential scanning calorimetry (DSC) at the same temperature. The extent of the phase transition depends on the DPPC concentration, with a lower DPPC concentration (and therefore a higher ice fraction), resulting in a higher degree of Lβ'-to-Gel III conversion. By comparing the data from this study with the literature data on the pressure/temperature Lβ'/Gel III phase boundary and the lamellar lattice constant of the Lβ' phase, the freeze-induced pressure is estimated to be approximately 0.2-2.6 kbar. The study introduces DPPC as a probe to detect a pressure increase during freezing, therefore addressing the gap between a theoretical possibility of protein destabilization by freeze-induced pressure and the current lack of methods to detect freeze-induced pressure. In addition, the observation of a freeze-induced phase transition in a phospholipid can improve the mechanistic understanding of factors that could disrupt the structure of lipid-based biopharmaceuticals, such as liposomes and mRNA vaccines, during freezing and thawing.

Microstructure and crystal order during freezing of supercooled water drops.

Supercooled water droplets are widely used to study supercooled water1,2, ice nucleation3-5 and droplet freezing6-11. Their freezing in the atmosphere affects the dynamics and climate feedback of clouds12,13 and can accelerate cloud freezing through secondary ice production14-17. Droplet freezing occurs at several timescales and length scales14,18 and is sufficiently stochastic to make it unlikely that two frozen drops are identical. Here we use optical microscopy and X-ray laser diffraction to investigate the freezing of tens of thousands of water microdrops in vacuum after homogeneous ice nucleation around 234-235 K. On the basis of drop images, we developed a seven-stage model of freezing and used it to time the diffraction data. Diffraction from ice crystals showed that long-range crystalline order formed in less than 1 ms after freezing, whereas diffraction from the remaining liquid became similar to that from quasi-liquid layers on premelted ice19,20. The ice had a strained hexagonal crystal structure just after freezing, which is an early metastable state that probably precedes the formation of ice with stacking defects8,9,18. The techniques reported here could help determine the dynamics of freezing in other conditions, such as drop freezing in clouds, or help understand rapid solidification in other materials.

Understanding the role of polymers on the nucleating behavior of water in dilute supercooled solutions.

Understanding the nucleation behavior of water in dilute polymeric solutions is quintessential for the development of suitable artificial ice recrystallization inhibition (IRI) agents. Although poly(vinyl alcohol) (PVA) is found to be one of the most potent biomimetic IRI agents, the molecular understanding of the nucleation behavior of water in the presence of PVA is still lacking. Here, we use molecular dynamics to elucidate the role of concentration, degree of supercooling, degree of polymerization, and amphiphilicity of PVA and PVA-like polymers on the homogeneous nucleation of water in dilute polymeric solutions using the seeding method. Using classical nucleation theory (CNT), our simulations indicate an increase in the chemical potential difference between ice and melt that favors ice nucleation. However, it also predicts a significant increase in the ice-melt interfacial energy that impedes nucleation. The relative increase in the interfacial energy dominates the increase in the chemical potential difference, which results in a decrease in the nucleation rate of water with an increase in the solute concentration. This study contradicts the previous simulation study that suggested the promotion of homogeneous ice nucleation by PVA and supports the experimental observations of the heterogeneous origins of ice nucleation. Our results also suggest the non-classical origins of ice nucleation in polymeric solutions and the limitation of the CNT in predicting heterogeneous ice nucleation in polymeric solutions.

Minimum in the pressure dependence of the interfacial free energy between ice Ih and water.

Despite the importance of ice nucleation, this process has been barely explored at negative pressures. Here, we study homogeneous ice nucleation in stretched water by means of molecular dynamics seeding simulations using the TIP4P/Ice model. We observe that the critical nucleus size, interfacial free energy, free energy barrier, and nucleation rate barely change between isobars from -2600 to 500 bars when they are represented as a function of supercooling. This allows us to identify universal empirical expressions for homogeneous ice nucleation in the pressure range from -2600 to 500 bars. We show that this universal behavior arises from the pressure dependence of the interfacial free energy, which we compute by means of the mold integration technique, finding a shallow minimum around -2000 bars. Likewise, we show that the change in the interfacial free energy with pressure is proportional to the excess entropy and the slope of the melting line, exhibiting in the latter a reentrant behavior also at the same negative pressure. Finally, we estimate the excess internal energy and the excess entropy of the ice Ih-water interface.

Improvements of the Double-Moment Bulk Cloud Microphysics Scheme in the Nonhydrostatic Icosahedral Atmospheric Model (NICAM)

Abstract This study revises the collisional growth, heterogeneous ice nucleation, and homogeneous ice nucleation processes in a double-moment bulk cloud microphysics scheme implemented in the Nonhydrostatic Icosahedral Atmospheric Model (NICAM). The revised cloud microphysical processes are tested by 10-day global simulations with a horizontal resolution of 14 km. It is found that both the aggregation of cloud ice with smaller diameters and the graupel production by riming are overestimated in the current schemes. A new method that numerically integrates the collection kernel solves this issue, and consequently, the lifetime of cloud ice is reasonably extended in reference to satellite observations. In addition, the results indicate that a reduction in graupel modulates the convective intensity, particularly in intense rainfall systems. The revision of both heterogeneous and homogeneous ice nucleation significantly increases the production rate of cloud ice number concentration. With these revisions, the new version of the cloud microphysics scheme successfully improves outgoing longwave radiation, particularly over the intertropical convergence zone, in reference to satellite observations. Therefore, the revisions are beneficial for both long-term climate simulations and representing the structure of severe storms. Significance Statement Very high-resolution global atmospheric models have been developed to simultaneously address global climate and regional weather. In general, cloud microphysics schemes used in such global models are introduced from regional weather forecasting models to realistically represent mesoscale cloud systems. However, a cloud microphysics scheme that was originally developed with the aim of weather forecasting can cause unexpected errors in global climate simulations because such a cloud microphysics scheme is not designed for interdisciplinary usage across spatiotemporal scales. This study focuses on systematic model biases in evaluating the terminal velocity of ice cloud particles and proposes a method to accurately calculate the growth rate of ice cloud particles. Improvements in ice cloud modeling successfully reduce model biases in the global energy budget. In addition, the internal structure of intense rainfall systems is modified using the new cloud model. Therefore, improvements in ice cloud modeling could further increase the reliability of weather forecasting, seasonal prediction, and climate projection.

Does liquid-liquid phase separation impact ice nucleation in mixed polyethylene glycol and ammonium sulfate droplets?

Particles can undergo different phase transitions in the atmosphere including deliquescence, liquid-liquid phase separation (LLPS), melting, and freezing. In this study, phase transitions of particles/droplets containing polyethylene glycol with a molar mass of 400 g mol-1 (PEG400) and ammonium sulfate (AS), i.e., PEG400-AS particles/droplets, were investigated at different organic-to-inorganic dry mass ratios (OIRs) under typical tropospheric temperatures and water activities (aw). The investigated droplets (60-100 μm) with or without LLPS in the closed system froze through homogeneous ice nucleation. At temperatures lower than 200 K, multiple ice nucleation events were observed within the same individual droplets at low aw. Droplets with and without LLPS shared similar lambda values at the same OIR according to the lambda approach indicating they form ice through the same mechanism. A parameterization of lambda values was provided which can be used to predict freezing temperature of aqueous PEG400-AS droplets. We found that adding AS reduces the temperature dependence of aw in aqueous PEG400 droplets. Assuming incorrectly that aw is temperature-independent for a constant droplet composition leads to a deviation between the experimental determined ice nucleation rate coefficients for droplets at OIR > 1 and the predicted values by the water-activity-based ice nucleation theory. We proposed a parameterization of temperature dependence of aw to minimize the deviations of the measured melting temperatures and nucleation rate coefficients from the corresponding predictions for aqueous PEG400-AS system.

Ice-nucleating agents in sea spray aerosol identified and quantified with a holistic multimodal freezing model.

Sea spray aerosol (SSA) is a widely recognized important source of ice-nucleating particles (INPs) in the atmosphere. However, composition-specific identification, nucleation processes, and ice nucleation rates of SSA-INPs have not been well constrained. Microspectroscopic characterization of ambient and laboratory-generated SSA confirms that water-borne exudates from planktonic microorganisms composed of a mixture of proteinaceous and polysaccharidic compounds act as ice-nucleating agents (INAs). These data and data from previously published mesocosm and wave channel studies are subsequently used to further develop the stochastic freezing model (SFM) producing ice nucleation rate coefficients for SSA-INPs. The SFM simultaneously predicts immersion freezing and deposition and homogeneous ice nucleation by SSA particles under tropospheric conditions. Predicted INP concentrations agree with ambient and laboratory measurements. In addition, this holistic freezing model is independent of the source and exact composition of the SSA particles, making it well suited for implementation in cloud and climate models.

The Microfluidic Ice Nuclei Counter Zürich (MINCZ): a platform for homogeneous and heterogeneous ice nucleation

Abstract. Ice nucleation in the atmosphere is the precursor to important processes that determine cloud properties and lifetime. Computational models that are used to predict weather and project future climate changes require parameterizations of both homogeneous nucleation (i.e. in pure water) and heterogeneous nucleation (i.e. catalysed by ice-nucleating particles, INPs). Microfluidic systems have gained momentum as a tool for obtaining such parameterizations and gaining insight into the stochastic and deterministic contributions to ice nucleation. To overcome the shortcomings of polydimethylsiloxane (PDMS) microfluidic devices with regard to temperature uncertainty and droplet instability due to continuous water adsorption by PDMS, we have developed a new instrument: the Microfluidic Ice Nuclei Counter Zürich (MINCZ). In MINCZ, droplets with a diameter of 75 µm are generated using a PDMS chip, and hundreds of these droplets are then stored in fluoropolymer tubing that is relatively impermeable to water and solvents. Droplets within the tubing are cooled in an ethanol bath. We validate MINCZ by measuring the homogeneous freezing temperatures of water droplets and the heterogeneous freezing temperatures of aqueous suspensions containing microcline, a common and effective INP in the atmosphere. We obtain results with a high accuracy of 0.2 K in measured droplet temperature. Pure water droplets with a diameter of 75 µm freeze at a median temperature of 237.3 K with a standard deviation of 0.1 K. Additionally, we perform several freeze–thaw cycles. In the future, MINCZ will be used to investigate the freezing behaviour of INPs, motivated by a need for better-constrained parameterizations of ice nucleation in weather and climate models, wherein the presence or absence of ice influences cloud optical properties and precipitation formation.

Homogeneous Freezing Events Sampled in the Tropical Tropopause Layer

AbstractHigh‐frequency (20 Hz) aircraft measurements of tropical tropopause layer (TTL) cirrus and humidity are used to examine recent homogeneous freezing ice nucleation events. Several localized regions with peak ice concentrations greater than 10 cm−3 are documented. These high ice concentrations are almost certainly generated by homogeneous freezing of aqueous aerosols. The high‐frequency data reveals considerable structure in the cloud properties and humidity at along‐track scales as short as 8.5 m. Simulations of vapor depletion by growing ice crystals are used to assess the time since nucleation in these high ice concentration patches. Comparisons between observed and simulated dependence of supersaturation on ice concentration indicate the nucleation events occurred within minutes (sometimes only a few minutes) of the aircraft sampling. The infrequency and short ages of the events suggest that the high ice concentrations do not persist for long times, but they may still be important for TTL cirrus microphysical properties by providing a source of ice crystals that can lead to extensive, persistent clouds with lower ice concentrations. We have also used the extensive TTL measurements provided by the high‐altitude aircraft campaigns to evaluate the threshold supersaturation for homogeneous freezing. Peak supersaturations observed are consistent with recent laboratory experiments indicating that ice saturation ratios of about 1.75–1.95 are required for homogeneous freezing of aqueous aerosols at temperatures of 185–200 K.

Evidence for Anthropogenic Organic Aerosols Contributing to Ice Nucleation

AbstractThe role of organic aerosols (OA) as ice nucleating particles (INPs) deserves attention because of their high atmospheric abundance. The low concentration of INPs poses challenges in identifying the ice nucleation (IN) of OA among a mix of aerosol types in ambient environment. This study coupled a catalytic stripper system (350°C heating) with a continuous flow diffusion chamber to online investigate the immersion INPs of ambient particles at −30°C at a suburban site. Significant reduction (71 ± 25%) of INP concentrations after evaporation suggested that INPs can be significantly contributed by volatile OA. In addition, nonvolatile OA were more efficient INPs than black carbon. Oxygenated OA by photooxidation and lower ambient promoted the IN activity at noon, when the OA may be more viscous. These results hereby present the first field evidence that OA in anthropogenically influenced regions can be efficient INPs well above the homogeneous IN temperature.

Homogeneous ice nucleation rates for mW and TIP4P/ICE models through Lattice Mold calculations.

Freezing of water is the most common liquid-to-crystal phase transition on Earth; however, despite its critical implications on climate change and cryopreservation among other disciplines, its characterization through experimental and computational techniques remains elusive. In this work, we make use of computer simulations to measure the nucleation rate (J) of water at normal pressure under different supercooling conditions, ranging from 215 to 240K. We employ two different water models: mW, a coarse-grained potential for water, and TIP4P/ICE, an atomistic nonpolarizable water model that provides one of the most accurate representations of the different ice phases. To evaluate J, we apply the Lattice Mold technique, a computational method based on the use of molds to induce the nucleus formation from the metastable liquid under conditions at which observing spontaneous nucleation would be unfeasible. With this method, we obtain estimates of the nucleation rate for ice Ih and Ic and a stacking mixture of ice Ih/Ic, reaching consensus with most of the previously reported rates, although differing with some others. Furthermore, we confirm that the predicted nucleation rates obtained by the TIP4P/ICE model are in better agreement with experimental data than those obtained through the mW potential. Taken together, our study provides a reliable methodology to measure nucleation rates in a simple and computationally efficient manner that contributes to benchmarking the freezing behavior of two popular water models.

Mechanism for the Efficient Homogeneous Nucleation of Ice in a Weakly Ionized, Ultracold Plasma

It is proposed that the rapid observed homogeneous nucleation of ice dust in a cold, weakly ionized plasma depends on the formation of hydroxide (OH−) by fast electrons impacting water molecules. These OH− ions attract neutral water molecules because of the high dipole moment of the water molecules and so hydrates of the form (OH)−(H2O) n are formed. The hydrates continuously grow in the cold environment to become macroscopic ice grains. These ice grains are negatively charged as a result of electron impact and so continue to attract water molecules. Because hydroxide is a negative ion, unlike positive ions, it does not suffer recombination loss from collision with plasma electrons. Recombination with positive ions is minimal because positive ions are few in number (weak ionization) and slow-moving as result of being in thermal equilibrium with the cold background gas.

Homogeneous ice nucleation in an ab initio machine-learning model of water

Molecular simulations have provided valuable insight into the microscopic mechanisms underlying homogeneous ice nucleation. While empirical models have been used extensively to study this phenomenon, simulations based on first-principles calculations have so far proven prohibitively expensive. Here, we circumvent this difficulty by using an efficient machine-learning model trained on density-functional theory energies and forces. We compute nucleation rates at atmospheric pressure, over a broad range of supercoolings, using the seeding technique and systems of up to hundreds of thousands of atoms simulated with ab initio accuracy. The key quantity provided by the seeding technique is the size of the critical cluster (i.e., a size such that the cluster has equal probabilities of growing or melting at the given supersaturation), which is used together with the equations of classical nucleation theory to compute nucleation rates. We find that nucleation rates for our model at moderate supercoolings are in good agreement with experimental measurements within the error of our calculation. We also study the impact of properties such as the thermodynamic driving force, interfacial free energy, and stacking disorder on the calculated rates.

Effective radiative forcing of anthropogenic aerosols in E3SM version 1: historical changes, causality, decomposition, and parameterization sensitivities

Abstract. The effective radiative forcing of anthropogenic aerosols (ERFaer) is an important measure of the anthropogenic aerosol effects simulated by a global climate model. Here we analyze ERFaer simulated by the E3SM version 1 (E3SMv1) atmospheric model using both century-long free-running atmosphere–land simulations and short nudged simulations. We relate the simulated ERFaer to characteristics of the aerosol composition and optical properties, and we evaluate the relationships between key aerosol and cloud properties. In terms of historical changes from the year 1870 to 2014, our results show that the global mean anthropogenic aerosol burden and optical depth increase during the simulation period as expected, but the regional averages show large differences in the temporal evolution. The largest regional differences are found in the emission-induced evolution of the burden and optical depth of the sulfate aerosol: a strong decreasing trend is seen in the Northern Hemisphere high-latitude region after around 1970, while a continued increase is simulated in the tropics. The relationships between key aerosol and cloud properties (relative changes between pre-industrial and present-day conditions) also show evident changes after 1970, diverging from the linear relationships exhibited for the period of 1870–1969. In addition to the regional differences in the simulated relationships, a reduced sensitivity in cloud droplet number and other cloud properties to aerosol perturbations is seen when the aerosol perturbation is large. Consequently, the global annual mean ERFaer magnitude does not increase after around 1970. The ERFaer in E3SMv1 is relatively large compared to the recently published multi-model estimates; the primary reason is the large indirect aerosol effect (i.e., through aerosol–cloud interactions). Compared to other models, E3SMv1 features large relative changes in the cloud droplet effective radius in response to aerosol perturbations. Large sensitivity is also seen in the liquid cloud optical depth, which is determined by changes in both the effective radius and liquid water path. Aerosol-induced changes in liquid and ice cloud properties in E3SMv1 are found to have a strong correlation, as the evolution of anthropogenic sulfate aerosols affects both the liquid cloud formation and the homogeneous ice nucleation in cirrus clouds (that causes a large effect on longwave ERFaer). As suggested by a previous study, the large ERFaer appears to be one of the reasons why the model cannot reproduce the observed global mean temperature evolution in the second half of the 20th century. Sensitivity simulations are performed to understand which parameterization and/or parameter changes have a large impact on the simulated ERFaer. The ERFaer estimates in E3SMv1 for the shortwave and longwave components are sensitive to the parameterization changes in both liquid and ice cloud processes. When the parameterization of ice cloud processes is modified, the top-of-model forcing changes in the shortwave and longwave components largely offset each other, so the net effect is negligible. This suggests that, to reduce the magnitude of the net ERFaer, it would be more effective to reduce the anthropogenic aerosol effect through liquid or mixed-phase clouds.