Size‐fractionated filtration (SFF) is a direct method for estimating pigment concentration in various size classes. It is also common practice to infer the size structure of phytoplankton communities from diagnostic pigments estimated by high‐performance liquid chromatography (HPLC). In this paper, the three‐component model of Brewin et al. (2010) was fitted to coincident data from HPLC and from SFF collected along Atlantic Meridional Transect cruises. The model accounted for the variability in each data set, but the fitted model parameters differed for the two data sets. Both HPLC and SFF data supported the conceptual framework of the three‐component model, which assumes that the chlorophyll concentration in small cells increases to an asymptotic maximum, beyond which further increase in chlorophyll is achieved by the addition of larger celled phytoplankton. The three‐component model was extended to a multicomponent model of size structure using observed relationships between model parameters and assuming that the asymptotic concentration that can be reached by cells increased linearly with increase in the upper bound on the cell size. The multicomponent model was verified using independent SFF data for a variety of size fractions and found to perform well (0.628 ≤ r ≤ 0.989) lending support for the underlying assumptions. An advantage of the multicomponent model over the three‐component model is that, for the same number of parameters, it can be applied to any size range in a continuous fashion. The multicomponent model provides a useful tool for studying the distribution of phytoplankton size structure at large scales.

Cell abundances of Prochlorococcus, Synechococcus, and autotrophic picoeukaryotes were estimated in surface waters using principal component analysis (PCA) of hyperspectral and multispectral remote-sensing reflectance data. This involved the development of models that employed multilinear correlations between cell abundances across the Atlantic Ocean and a combination of PCA scores and sea surface temperatures. The models retrieve high Prochlorococcus abundances in the Equatorial Convergence Zone and show their numerical dominance in oceanic gyres, with decreases in Prochlorococcus abundances towards temperate waters where Synechococcus flourishes, and an emergence of picoeukaryotes in temperate waters. Fine-scale in-situ sampling across ocean fronts provided a large dynamic range of measurements for the training dataset, which resulted in the successful detection of fine-scale Synechococcus patches. Satellite implementation of the models showed good performance (R² > 0.50) when validated against in-situ data from six Atlantic Meridional Transect cruises. The improved relative performance of the hyperspectral models highlights the importance of future high spectral resolution satellite instruments, such as the NASA PACE mission’s Ocean Color Instrument, to extend our spatiotemporal knowledge about ecologically relevant phytoplankton assemblages.