## Appendix A

Below are shown the speed profiles of the Artemis Urban and Artemis Motorway cycles.

<figure><img src="image_14.png" /><figcaption>**Figure A1.** Speed in km h⁻¹ during the Artemis Urban cycle (a) and the Artemis Motorway cycle (b), with the different types of driving found under those conditions.</figcaption></figure>

## Appendix B

Below are listed the constants taken for the calculation of $β(D_p)$.

- $k_B = 1.381 \times 10^{-23} \text{ J K}^{-1}$ the Boltzmann constant

- T (K) the temperature in the chamber for each experiment

- $\mu = 1.8 \times 10^{-5} \text{ kg m}^{-1} \text{ s}^{-1}$ the viscosity of air

- $\rho_p = 1.2 \text{ g cm}^{-3}$ the particle density

- $g = 9.81 \text{ m s}^{-2}$ the g force

- $\lambda = 6.51 \text{ nm}$ the mean-free path of air

## Appendix C

<table><caption>**Table C1.** Emission factors in $\text{mg km}^{-1}$ of linear (n-) and branched (b-) alkanes with carbon numbers below between 12 and 22 (C₁₂–C₂₂) and of naphthalene, cycloalkanes and aromatics measured with the ATD-GC-MS method. The sum of those EFs gives the IVOC EFs. Emission factors of n- and b-alkanes with carbon number above 22. Emission factors of NMHCs measured by flame ionization detection. Emissions below the quantification limit are indicated as “< QL”. Ratio of IVOC / NMHC expressed as percentage of NMHCs. Results are shown for vehicles D1 (Euro 3), D2 (Euro 4), D3 (Euro 5 add DPF), D5 (Euro 5 cat DPF) and D6 (Euro 6 add DPF and SCR) under both UC and MW conditions.</caption><thead><tr><th>Vehicle</th><th>D1</th><th>D2</th><th>D3 (add DPF)</th><th>D5 (cat DPF)</th><th>D6 (add DPF and SCR)</th></tr><tr><th>Cycle</th><th>UC</th><th>MW</th><th>MW</th><th>UC</th><th>MW</th><th>UC</th><th>MW</th></tr></thead><tbody><tr><td>n/b- alkanes</td><td>1.05 ± 0.31</td><td>1.25 ± 0.08</td><td>0.19 ± 0.03</td><td>0.55 ± 0.48</td><td>0.12 ± 0.02</td><td>0.02 ± 0.01</td><td>0.72 ± 0.10</td><td>0.65 ± 0.68</td><td>0.04 ± 0.04</td><td>0.02 ± 0.02</td></tr><tr><td>C₁₂–C₂₂ (mg km⁻¹)</td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Naphthalene (mg km⁻¹)</td><td>0.03 ± 0.03</td><td>0.06 ± 0.02</td><td>0.04 ± 0.01</td><td>0.09 ± 0.05</td><td>&lt; QL</td><td>&lt; QL</td><td>0.01 ± 0.01</td><td>&lt; QL</td><td>&lt; QL</td><td>&lt; QL</td></tr><tr><td>Cycloalkanes (mg km⁻¹)</td><td>0.2 ± 0.10</td><td>0.22 ± 0.01</td><td>0.05 ± 0.04</td><td>0.16 ± 0.16</td><td>&lt; QL</td><td>&lt; QL</td><td>0.29 ± 0.06</td><td>0.08 ± 0.12</td><td>&lt; QL</td><td>&lt; QL</td></tr><tr><td>Aromatics (mg km⁻¹)</td><td>0.04 ± 0.49</td><td>0.05 ± 0.13</td><td>0.23 ± 0.40</td><td>0.12 ± 0.74</td><td>&lt; QL</td><td>&lt; QL</td><td>0.04 ± 0.17</td><td>0.01 ± 0.82</td><td>&lt; QL</td><td>&lt; QL</td></tr><tr><td>IVOCs (mg km⁻¹)</td><td>1.32 ± 0.93</td><td>1.58 ± 0.24</td><td>0.5 ± 0.48</td><td>0.92 ± 1.42</td><td>0.12 ± 0.04</td><td>0.02 ± 0.01</td><td>1.06 ± 0.34</td><td>0.74 ± 1.62</td><td>0.04 ± 0.08</td><td>0.02 ± 0.04</td></tr><tr><td>n/b- alkanes</td><td>1.56 ± 1.26</td><td>1.27 ± 1.35</td><td>0.26 ± 0.30</td><td>0.66 ± 0.01</td><td>0.35 ± 0.06</td><td>0.29 ± 0.43</td><td>1.46 ± 1.47</td><td>2.63 ± 3.17</td><td>0.17 ± 0.12</td><td>0.2 ± 0.24</td></tr><tr><td>C>22 (mg km⁻¹)</td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>NMHCs (mg km⁻¹)</td><td>102.93 ± 39.43</td><td>22.82 ± 2.79</td><td>52.31 ± 27.29</td><td>18.38 ± 2.29</td><td>22.68 ± 0.89</td><td>2.25 ± 0.53</td><td>113.37 ± 2.00</td><td>3.01 ± 4.14</td><td>5.18 ± 0.96</td><td>No data</td></tr><tr><td>IVOC / NMHC (%)</td><td>1.28 ± 0.48</td><td>6.91 ± 0.59</td><td>0.96 ± 0.77</td><td>5.00 ± 4.02</td><td>0.54 ± 0.09</td><td>0.88 ± 0.21</td><td>0.93 ± 0.15</td><td>24.73 ± 27.10</td><td>0.79 ± 0.78</td><td>No data</td></tr></tbody></table>

<footnote>* QL: quantification limit.</footnote>
## Appendix A

Below are shown the speed profiles of the Artemis Urban and Artemis Motorway cycles.

<figure><img src="image_14.png" /><figcaption>**Figure A1.** Speed in km h⁻¹ during the Artemis Urban cycle (a) and the Artemis Motorway cycle (b), with the different types of driving found under those conditions.</figcaption></figure>

## Appendix B

Below are listed the constants taken for the calculation of $β(D_p)$.

- $k_B = 1.381 \times 10^{-23} \text{ J K}^{-1}$ the Boltzmann constant

- T (K) the temperature in the chamber for each experiment

- $\mu = 1.8 \times 10^{-5} \text{ kg m}^{-1} \text{ s}^{-1}$ the viscosity of air

- $\rho_p = 1.2 \text{ g cm}^{-3}$ the particle density

- $g = 9.81 \text{ m s}^{-2}$ the g force

- $\lambda = 6.51 \text{ nm}$ the mean-free path of air

## Appendix C

<table><caption>**Table C1.** Emission factors in $\text{mg km}^{-1}$ of linear (n-) and branched (b-) alkanes with carbon numbers below between 12 and 22 (C₁₂–C₂₂) and of naphthalene, cycloalkanes and aromatics measured with the ATD-GC-MS method. The sum of those EFs gives the IVOC EFs. Emission factors of n- and b-alkanes with carbon number above 22. Emission factors of NMHCs measured by flame ionization detection. Emissions below the quantification limit are indicated as “< QL”. Ratio of IVOC / NMHC expressed as percentage of NMHCs. Results are shown for vehicles D1 (Euro 3), D2 (Euro 4), D3 (Euro 5 add DPF), D5 (Euro 5 cat DPF) and D6 (Euro 6 add DPF and SCR) under both UC and MW conditions.</caption><thead><tr><th>Vehicle</th><th>D1</th><th>D2</th><th>D3 (add DPF)</th><th>D5 (cat DPF)</th><th>D6 (add DPF and SCR)</th></tr><tr><th>Cycle</th><th>UC</th><th>MW</th><th>MW</th><th>UC</th><th>MW</th><th>UC</th><th>MW</th></tr></thead><tbody><tr><td>n/b- alkanes</td><td>1.05 ± 0.31</td><td>1.25 ± 0.08</td><td>0.19 ± 0.03</td><td>0.55 ± 0.48</td><td>0.12 ± 0.02</td><td>0.02 ± 0.01</td><td>0.72 ± 0.10</td><td>0.65 ± 0.68</td><td>0.04 ± 0.04</td><td>0.02 ± 0.02</td></tr><tr><td>C₁₂–C₂₂ (mg km⁻¹)</td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>Naphthalene (mg km⁻¹)</td><td>0.03 ± 0.03</td><td>0.06 ± 0.02</td><td>0.04 ± 0.01</td><td>0.09 ± 0.05</td><td>&lt; QL</td><td>&lt; QL</td><td>0.01 ± 0.01</td><td>&lt; QL</td><td>&lt; QL</td><td>&lt; QL</td></tr><tr><td>Cycloalkanes (mg km⁻¹)</td><td>0.2 ± 0.10</td><td>0.22 ± 0.01</td><td>0.05 ± 0.04</td><td>0.16 ± 0.16</td><td>&lt; QL</td><td>&lt; QL</td><td>0.29 ± 0.06</td><td>0.08 ± 0.12</td><td>&lt; QL</td><td>&lt; QL</td></tr><tr><td>Aromatics (mg km⁻¹)</td><td>0.04 ± 0.49</td><td>0.05 ± 0.13</td><td>0.23 ± 0.40</td><td>0.12 ± 0.74</td><td>&lt; QL</td><td>&lt; QL</td><td>0.04 ± 0.17</td><td>0.01 ± 0.82</td><td>&lt; QL</td><td>&lt; QL</td></tr><tr><td>IVOCs (mg km⁻¹)</td><td>1.32 ± 0.93</td><td>1.58 ± 0.24</td><td>0.5 ± 0.48</td><td>0.92 ± 1.42</td><td>0.12 ± 0.04</td><td>0.02 ± 0.01</td><td>1.06 ± 0.34</td><td>0.74 ± 1.62</td><td>0.04 ± 0.08</td><td>0.02 ± 0.04</td></tr><tr><td>n/b- alkanes</td><td>1.56 ± 1.26</td><td>1.27 ± 1.35</td><td>0.26 ± 0.30</td><td>0.66 ± 0.01</td><td>0.35 ± 0.06</td><td>0.29 ± 0.43</td><td>1.46 ± 1.47</td><td>2.63 ± 3.17</td><td>0.17 ± 0.12</td><td>0.2 ± 0.24</td></tr><tr><td>C>22 (mg km⁻¹)</td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td><td></td></tr><tr><td>NMHCs (mg km⁻¹)</td><td>102.93 ± 39.43</td><td>22.82 ± 2.79</td><td>52.31 ± 27.29</td><td>18.38 ± 2.29</td><td>22.68 ± 0.89</td><td>2.25 ± 0.53</td><td>113.37 ± 2.00</td><td>3.01 ± 4.14</td><td>5.18 ± 0.96</td><td>No data</td></tr><tr><td>IVOC / NMHC (%)</td><td>1.28 ± 0.48</td><td>6.91 ± 0.59</td><td>0.96 ± 0.77</td><td>5.00 ± 4.02</td><td>0.54 ± 0.09</td><td>0.88 ± 0.21</td><td>0.93 ± 0.15</td><td>24.73 ± 27.10</td><td>0.79 ± 0.78</td><td>No data</td></tr></tbody></table>

<footnote>* QL: quantification limit.</footnote>
## Appendix D

Figure D1a and b show two examples of [BC] evolutions and decay fits. Figure D1a is an example of an evolution well fitted by a first-order exponential decay. Figure D1b shows an evolution not well fitted by a first-order exponential decay. For instance, the fitted initial concentration is 12.1 µg m⁻³, whereas the actual initial concentration is 23.2 µg m⁻³. This means that this fit would induce an error of 48 % on the initial concentration. However, the second-order exponential decay matches very well the measured values.

## Appendix E

To verify how well [PM] corrections from steps 1 and 2 agree, the average relative agreement between [PM]step 1corrected(t) and [PM]step 1corrected(t) is computed as given in Eq. (E1).

Agreement(%) = 100

$$ -\frac{1}{n} \times \left( \sum_{i=0}^{n} \frac{\left| [PM]_{corrected}^{step 1}(t_i) - [PM]_{corrected}^{step 2}(t_i) \right|}{[PM]_{corrected}^{step 1}(t_i)} \right) \times 100 \quad (E1) $$

<figure><img src="image_15.png" /><figcaption>Figure D1. Evolution of the measured BC concentration (white circles) for the G4-DI vehicle under MW conditions (a) and the D4-DPF vehicle under UC conditions (b). The curve is fitted with a first-order exponential decay (blue) in both cases and with a second-order exponential decay (red) in panel (b).</figcaption></figure>
## Appendix D

Figure D1a and b show two examples of [BC] evolutions and decay fits. Figure D1a is an example of an evolution well fitted by a first-order exponential decay. Figure D1b shows an evolution not well fitted by a first-order exponential decay. For instance, the fitted initial concentration is 12.1 µg m⁻³, whereas the actual initial concentration is 23.2 µg m⁻³. This means that this fit would induce an error of 48 % on the initial concentration. However, the second-order exponential decay matches very well the measured values.

## Appendix E

To verify how well [PM] corrections from steps 1 and 2 agree, the average relative agreement between [PM]step 1corrected(t) and [PM]step 1corrected(t) is computed as given in Eq. (E1).

Agreement(%) = 100

$$ -\frac{1}{n} \times \left( \sum_{i=0}^{n} \frac{\left| [PM]_{corrected}^{step 1}(t_i) - [PM]_{corrected}^{step 2}(t_i) \right|}{[PM]_{corrected}^{step 1}(t_i)} \right) \times 100 \quad (E1) $$

<figure><img src="image_15.png" /><figcaption>Figure D1. Evolution of the measured BC concentration (white circles) for the G4-DI vehicle under MW conditions (a) and the D4-DPF vehicle under UC conditions (b). The curve is fitted with a first-order exponential decay (blue) in both cases and with a second-order exponential decay (red) in panel (b).</figcaption></figure>
## Appendix F

Figure F1 shows uncorrected [PM] measurements (black crosses) and corrected [PM] for the Euro 3 (red) and Euro 4 (blue) vehicles under UC (triangles) and MW (circles) conditions. Figure F1a, b and c show “long” evolutions for which corrected [PM] reaches its maximum after several hours (> 400 min). Those figures correspond to the points on the upper left-hand side of Fig. 9a, with lower initial particle surface. Figure F1d shows a “rapid” [PM] evolution for which the corrected concentration reaches its maximum in tan 105 min. It corresponds to one of the points on the lower right-hand side of Fig. 9a, with a higher initial particle surface. For the “long” evolution of Fig. F1a, the measured concentration increases during 80 min. After that, it slightly decreases, with a decrease rate smaller than that of BC (hence the continuous increase in corrected [PM]). Figure F1b and c show that measured [PM] steadily increases during 295 to 320 min. It then remains pretty constant. Considering the fact that all of these measured concentrations (Fig. F1a to c) are subject to leakage and wall deposition, the fact that they increase during up to 6 h and then mostly remain constant shows that continuous increase in [PM] is possible during several hours. Therefore, the continuous increases in corrected [PM] observed in Figs. 8 and 9 are not likely to be an artifact induced by the correction algorithm. These increases are obviously more important and longer on corrected concentrations, but this is normal as leakage and wall deposition, which both lower [PM], are corrected. Moreover, the “rapid” evolution of Fig. F1d lasts 80 min for measured [PM], with an increase rate of 12% h⁻¹. These values indicate that there is indeed a rapid and significant increase in [PM] during the beginning of the evolution. Then, concentrations start slowly decreasing before reaching a steady decrease rate (similarly to that of BC). This is consistent with the evolution of the corrected concentration, which increases significantly and then increases more slightly before it reaches a maximum and remains constant. Here again, it seems that the significant and rapid increase observed for corrected [PM] of Fig. F1d is not an artifact induced by the correction method.

## Appendix G

The effective saturation concentrations of n-alkanes up to C₃₂ are obtained with the method described in Lu et al. (2018) for VOCs (C>12), IVOCs (C₁₂–C₂₂) and SVOCs (C₂₃–C₃₂). Using Eq. (14.43) from Seinfeld and Pandis (2016), the fraction in particle phase is computed for two conditions of initial [PM] typical of significant [PM] increase observed in Fig. 9 (200 and 2500 µg m⁻³). The organic aerosol concentration [OA] is estimated to range roughly between 2% and 80% of [PM]. This range is based on studies giving the ratio [PM] / [OA] or the ratio EC/OC, which cover a wide range of values (Kostenidou et al., 2021; May et al.,

<figure><img src="image_16.png" /><figcaption>**Figure F1.** Evolution of the corrected PM concentrations for the Euro 3 vehicle (red) and Euro 4 vehicle (blue) under both UC (triangles) and MW (circles) conditions. Panels (a), (b) and (c) represent long increases, whereas panel (d) represents a short increase. The corrected concentrations are compared to the measured (e.g., un-corrected) PM concentrations (black crosses). Labels give for each evolution (measured or corrected) the time at which [PM] reaches its maximum as well as the associated hourly increase.</figcaption></figure>

2014). The wide range is caused by several parameters, such as measurement technique, experimental conditions, driving conditions, and vehicle type (motorization and aftertreatment technologies). Results are given in Fig. G1 as areas delimited by the lower (2%) and upper (80%) estimates of [PM] / [OA]. The grey area is for initial [PM] = 200 µg m⁻³ (with [OA] ranging from 4 to 160 µg m⁻³), and the hatched blue area is for initial [PM] = 2500 µg m⁻³ (with [OA] ranging from 50 to 160 µg m⁻³). Also, in this study, the Euro 3 and Euro 4 vehicles have differences between initial concentrations of PM and BC of about 69.6% of initial [PM]. This indicates that [OA] could represent up to 69% of [PM]. This value is used for another estimation of [OA]. The associated fractions are shown in Fig. G1 for initial [PM] = 200 µg m⁻³ (grey line, associated [OA] = 138 µg m⁻³) and for initial [PM] = 2500 µg m⁻³ (dashed blue line, associated [OA] = 1725 µg m⁻³).

For the condition with initial [PM] = 200 µg m⁻³, the percentage of n-alkanes IVOCs present in the particle phase ranges from 0.8% to 13.7% for [OA] estimated as 2% and 80% of [PM], respectively. The percentage of n-alkanes SVOCs in the particle phase ranges from 85.5% to 98.7%, respectively. For the estimation with [OA] = 69% of [PM], 12.7% of n-alkanes IVOCs and 98.5% of n-alkanes SVOCs are in the particle phase.
## Appendix F

Figure F1 shows uncorrected [PM] measurements (black crosses) and corrected [PM] for the Euro 3 (red) and Euro 4 (blue) vehicles under UC (triangles) and MW (circles) conditions. Figure F1a, b and c show “long” evolutions for which corrected [PM] reaches its maximum after several hours (> 400 min). Those figures correspond to the points on the upper left-hand side of Fig. 9a, with lower initial particle surface. Figure F1d shows a “rapid” [PM] evolution for which the corrected concentration reaches its maximum in tan 105 min. It corresponds to one of the points on the lower right-hand side of Fig. 9a, with a higher initial particle surface. For the “long” evolution of Fig. F1a, the measured concentration increases during 80 min. After that, it slightly decreases, with a decrease rate smaller than that of BC (hence the continuous increase in corrected [PM]). Figure F1b and c show that measured [PM] steadily increases during 295 to 320 min. It then remains pretty constant. Considering the fact that all of these measured concentrations (Fig. F1a to c) are subject to leakage and wall deposition, the fact that they increase during up to 6 h and then mostly remain constant shows that continuous increase in [PM] is possible during several hours. Therefore, the continuous increases in corrected [PM] observed in Figs. 8 and 9 are not likely to be an artifact induced by the correction algorithm. These increases are obviously more important and longer on corrected concentrations, but this is normal as leakage and wall deposition, which both lower [PM], are corrected. Moreover, the “rapid” evolution of Fig. F1d lasts 80 min for measured [PM], with an increase rate of 12 % h⁻¹. These values indicate that there is indeed a rapid and significant increase in [PM] during the beginning of the evolution. Then, concentrations start slowly decreasing before reaching a steady decrease rate (similarly to that of BC). This is consistent with the evolution of the corrected concentration, which increases significantly and then increases more slightly before it reaches a maximum and remains constant. Here again, it seems that the significant and rapid increase observed for corrected [PM] of Fig. F1d is not an artifact induced by the correction method.

## Appendix G

The effective saturation concentrations of n-alkanes up to C₃₂ are obtained with the method described in Lu et al. (2018) for VOCs (C>12), IVOCs (C₁₂–C₂₂) and SVOCs (C₂₃–C₃₂). Using Eq. (14.43) from Seinfeld and Pandis (2016), the fraction in particle phase is computed for two conditions of initial [PM] typical of significant [PM] increase observed in Fig. 9 (200 and 2500 µg m⁻³). The organic aerosol concentration [OA] is estimated to range roughly between 2 % and 80 % of [PM]. This range is based on studies giving the ratio [PM] / [OA] or the ratio EC/OC, which cover a wide range of values (Kostenidou et al., 2021; May et al.,

<figure><img src="image_16.png" /><figcaption>**Figure F1.** Evolution of the corrected PM concentrations for the Euro 3 vehicle (red) and Euro 4 vehicle (blue) under both UC (triangles) and MW (circles) conditions. Panels (a), (b) and (c) represent long increases, whereas panel (d) represents a short increase. The corrected concentrations are compared to the measured (e.g., un-corrected) PM concentrations (black crosses). Labels give for each evolution (measured or corrected) the time at which [PM] reaches its maximum as well as the associated hourly increase.</figcaption></figure>

2014). The wide range is caused by several parameters, such as measurement technique, experimental conditions, driving conditions, and vehicle type (motorization and aftertreatment technologies). Results are given in Fig. G1 as areas delimited by the lower (2 %) and upper (80 %) estimates of [PM] / [OA]. The grey area is for initial [PM] = 200 µg m⁻³ (with [OA] ranging from 4 to 160 µg m⁻³), and the hatched blue area is for initial [PM] = 2500 µg m⁻³ (with [OA] ranging from 50 to 160 µg m⁻³). Also, in this study, the Euro 3 and Euro 4 vehicles have differences between initial concentrations of PM and BC of about 69.6 % of initial [PM]. This indicates that [OA] could represent up to 69 % of [PM]. This value is used for another estimation of [OA]. The associated fractions are shown in Fig. G1 for initial [PM] = 200 µg m⁻³ (grey line, associated [OA] = 138 µg m⁻³) and for initial [PM] = 2500 µg m⁻³ (dashed blue line, associated [OA] = 1725 µg m⁻³).

For the condition with initial [PM] = 200 µg m⁻³, the percentage of n-alkanes IVOCs present in the particle phase ranges from 0.8 % to 13.7 % for [OA] estimated as 2 % and 80 % of [PM], respectively. The percentage of n-alkanes SVOCs in the particle phase ranges from 85.5 % to 98.7 %, respectively. For the estimation with [OA] = 69 % of [PM], 12.7 % of n-alkanes IVOCs and 98.5 % of n-alkanes SVOCs are in the particle phase.
<figure><img src="image_17.png" /></figure>

**Figure G1.** Particle fraction at *T* = 298 K of n-alkanes (VOCs, IVOCs and SVOCs), in percentage, with carbon number between 2 and 32. The repartition is given assuming two initial PM concentrations of 200 µg m⁻³ (grey) and 2500 µg m⁻³ (blue), typical of significant [PM] increase. *X*<sub>p</sub> is computed with different estimates of organic aerosol concentrations [OA], ranging from 2 % to 80 % of initial [PM] (grey area and blue hatched area, respectively). It is also computed assuming that [OA] = 69 % of initial [PM], with initial [PM] of 200 µg m⁻³ (continuous grey line) and 2500 µg m⁻³ (dashed blue line).

For the condition with initial [PM] = 2500 µg m⁻³, the percentage of n-alkanes IVOCs present in the particle phase ranges from 6.7% to 34.0% for [OA] estimated as 2% and 80% of [PM], respectively. The percentage of n-alkanes SVOCs in the particle phase ranges from 96.5% to 99.9%, respectively. For the estimation with [OA] = 69% of [PM], 32.7% of n-alkanes IVOCs and 99.9% of n-alkanes SVOCs are in the particle phase.

These results show that at such high particle concentrations, significant fractions of n-alkanes IVOCs and n-alkanes SVOCs could be present in the particle phase. Overall, it indicates that IVOCs can participate in the [PM] evolutions observed in Figs. 8 and 9, due to high PM concentrations and the presence of IVOCs (Fig. 6d) for the Euro 3 and Euro 4 vehicles. SVOCs can also be a significant contributor to [PM] evolutions.

## Appendix H

Figure H1 shows measured lognormal [PN] evolutions (e.g., not corrected) for two cycles concerned by continuous [PM] increase during several hours, as seen in Fig. 9. The cycles are from the two concerned vehicles: Euro 3 UC (Fig. H1a and b) and Euro 4 MW (Fig. H1c and d) conditions. On the left are presented the measured [PN] evolutions over the whole SMPS measurement range. On the right are presented the same data but with a focus on smaller diameters (up to 50 nm) and with a more adapted scale. It shows that under both conditions there is the presence of small particles (below 20 nm). Their concentrations show a slight decrease over the course of the experiments, but they are present until the end. They could come from growth (due to coagulation or condensation) of nucleation-mode particles. Their concentrations remaining quite constant could be because they are at the same time increasing (from growth of nucleation-mode particles) and decreasing (from their own coagulation). This phenomenon could partly explain the continuous [PM] increase observed in Figs. 8 and 9 for the Euro 3 and Euro 4 vehicles.
<figure><img src="image_17.png" /></figure>

**Figure G1.** Particle fraction at *T* = 298 K of n-alkanes (VOCs, IVOCs and SVOCs), in percentage, with carbon number between 2 and 32. The repartition is given assuming two initial PM concentrations of 200 µg m⁻³ (grey) and 2500 µg m⁻³ (blue), typical of significant [PM] increase. *X*<sub>p</sub> is computed with different estimates of organic aerosol concentrations [OA], ranging from 2 % to 80 % of initial [PM] (grey area and blue hatched area, respectively). It is also computed assuming that [OA] = 69 % of initial [PM], with initial [PM] of 200 µg m⁻³ (continuous grey line) and 2500 µg m⁻³ (dashed blue line).

For the condition with initial [PM] = 2500 µg m⁻³, the percentage of n-alkanes IVOCs present in the particle phase ranges from 6.7% to 34.0% for [OA] estimated as 2% and 80% of [PM], respectively. The percentage of n-alkanes SVOCs in the particle phase ranges from 96.5% to 99.9%, respectively. For the estimation with [OA] = 69% of [PM], 32.7% of n-alkanes IVOCs and 99.9% of n-alkanes SVOCs are in the particle phase.

These results show that at such high particle concentrations, significant fractions of n-alkanes IVOCs and n-alkanes SVOCs could be present in the particle phase. Overall, it indicates that IVOCs can participate in the [PM] evolutions observed in Figs. 8 and 9, due to high PM concentrations and the presence of IVOCs (Fig. 6d) for the Euro 3 and Euro 4 vehicles. SVOCs can also be a significant contributor to [PM] evolutions.

## Appendix H

Figure H1 shows measured lognormal [PN] evolutions (e.g., not corrected) for two cycles concerned by continuous [PM] increase during several hours, as seen in Fig. 9. The cycles are from the two concerned vehicles: Euro 3 UC (Fig. H1a and b) and Euro 4 MW (Fig. H1c and d) conditions. On the left are presented the measured [PN] evolutions over the whole SMPS measurement range. On the right are presented the same data but with a focus on smaller diameters (up to 50 nm) and with a more adapted scale. It shows that under both conditions there is the presence of small particles (below 20 nm). Their concentrations show a slight decrease over the course of the experiments, but they are present until the end. They could come from growth (due to coagulation or condensation) of nucleation-mode particles. Their concentrations remaining quite constant could be because they are at the same time increasing (from growth of nucleation-mode particles) and decreasing (from their own coagulation). This phenomenon could partly explain the continuous [PM] increase observed in Figs. 8 and 9 for the Euro 3 and Euro 4 vehicles.
<figure><img src="image_18.png" /></figure>

**Figure H1.** Measured PN distribution evolutions for the Euro 3 UC (a, b) and Euro 4 MW (c, d) conditions. The x axis gives the evolution time in minutes. The y axis gives the diameter in nanometers. The color scale gives the lognormal concentration. Panels (a) and (c) give the PN distributions for the whole SMPS measurement range. Panels (b) and (d) show the same cycles for the range 14 to 50 nm. The color scales are changed to see the smallest particles.

*Data availability.* All data from this study are available from the authors upon request.

*Author contributions.* YL, BD'A, CF, KS, CL and BV designed the research. YL, CL and BV performed and analyzed the characterization experiments. YL and BV performed and analyzed the emission and evolution experiments. CF, LF and BV performed the ATD-GCMS analysis. EK, BTR and BD'A contributed to the experimental setup and the experimental procedure. PT and PP drove the cars and helped with the experimental setup. BV synthesized all the data and wrote the paper with contributions from CL, VC, BD'A, EK, BTR, KS, CF and YL.

*Competing interests.* The contact author has declared that neither they nor their co-authors have any competing interests.

*Disclaimer.* Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

*Acknowledgements.* This work was supported by the ADEME CORTEA program with project MAESTRO.

*Financial support.* This research has been supported by the Agence de la Transition Écologique ADEME (grant no. 1766C0001).

*Review statement.* This paper was edited by Pierre Herckes and reviewed by three anonymous referees.
<figure><img src="image_18.png" /></figure>

**Figure H1.** Measured PN distribution evolutions for the Euro 3 UC (a, b) and Euro 4 MW (c, d) conditions. The x axis gives the evolution time in minutes. The y axis gives the diameter in nanometers. The color scale gives the lognormal concentration. Panels (a) and (c) give the PN distributions for the whole SMPS measurement range. Panels (b) and (d) show the same cycles for the range 14 to 50 nm. The color scales are changed to see the smallest particles.

*Data availability.* All data from this study are available from the authors upon request.

*Author contributions.* YL, BD'A, CF, KS, CL and BV designed the research. YL, CL and BV performed and analyzed the characterization experiments. YL and BV performed and analyzed the emission and evolution experiments. CF, LF and BV performed the ATD-GCMS analysis. EK, BTR and BD'A contributed to the experimental setup and the experimental procedure. PT and PP drove the cars and helped with the experimental setup. BV synthesized all the data and wrote the paper with contributions from CL, VC, BD'A, EK, BTR, KS, CF and YL.

*Competing interests.* The contact author has declared that neither they nor their co-authors have any competing interests.

*Disclaimer.* Publisher's note: Copernicus Publications remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

*Acknowledgements.* This work was supported by the ADEME CORTEA program with project MAESTRO.

*Financial support.* This research has been supported by the Agence de la Transition Écologique ADEME (grant no. 1766C0001).

*Review statement.* This paper was edited by Pierre Herckes and reviewed by three anonymous referees.
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Weitkamp, E. A., Sage, A. M., Pierce, J. R., Donahue, N. M., and Robinson, A. L.: Organic Aerosol Formation from Photochemical Oxidation of Diesel Exhaust in a Smog Chamber, Environ. Sci. Technol., 41, 6969–6975, https://doi.org/10.1021/es070193r, 2007.

Xu, R., Alam, M. S., Stark, C., and Harrison, R. M.: Behaviour of traffic emitted semi-volatile and intermediate volatility organic compounds within the urban atmosphere, Sci. Total Environ., 720, 137470, https://doi.org/10.1016/j.scitotenv.2020.137470, 2020.

Yeh, G. K. and Ziemann, P. J.: Gas-Wall Partitioning of Oxygenated Organic Compounds: Measurements, Structure–Activity Relationships, and Correlation with Gas Chromatographic Retention Factor, Aerosol Sci. Tech., 49, 727–738, https://doi.org/10.1080/02786826.2015.1068427, 2015.

Zhang, K. M. and Wexler, A. S.: Evolution of particle number distribution near roadways – Part I: analysis of aerosol dynamics and its implications for engine emission measurement, Atmos. Environ., 38, 6643–6653, https://doi.org/10.1016/j.atmosenv.2004.06.043, 2004.

Zhang, K. M., Wexler, A. S., Zhu, Y. F., Hinds, W. C., and Sioutas, C.: Evolution of particle number distribution near roadways. Part II: the “Road-to-Ambient” process, Atmos. Environ., 38, 6655–6665, https://doi.org/10.1016/j.atmosenv.2004.06.044, 2004.

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Zhang, X., Schwantes, R. H., McVay, R. C., Lignell, H., Coggon, M. M., Flagan, R. C., and Seinfeld, J. H.: Vapor wall deposition in Teflon chambers, Atmos. Chem. Phys., 15, 4197–4214, https://doi.org/10.5194/acp-15-4197-2015, 2015.

Zhao, Y., Nguyen, N. T., Presto, A. A., Hennigan, C. J., May, A. A., and Robinson, A. L.: Intermediate Volatility Organic Compound Emissions from On-Road Diesel Vehicles: Chemical Composition, Emission Factors, and Estimated Secondary Organic Aerosol Production, Environ. Sci. Technol., 49, 11516–11526, https://doi.org/10.1021/acs.est.5b02841, 2015.

Zhao, Y., Nguyen, N. T., Presto, A. A., Hennigan, C. J., May, A. A., and Robinson, A. L.: Intermediate Volatility Organic Compound Emissions from On-Road Gasoline Vehicles and Small Off-Road Gasoline Engines, Environ. Sci. Technol., 50, 4554–4563, https://doi.org/10.1021/acs.est.5b06247, 2016.

Zhao, Y., Lambe, A. T., Saleh, R., Saliba, G., and Robinson, A. L.: Secondary Organic Aerosol Production from Gasoline Vehicle Exhaust: Effects of Engine Technology, Cold Start, and Emission Certification Standard, Environ. Sci. Technol., 52, 1253–1261, https://doi.org/10.1021/acs.est.7b05045, 2018.

Zhu, J., Penner, J. E., Lin, G., Zhou, C., Xu, L., and Zhuang, B.: Mechanism of SOA formation determines magnitude of radiative effects, P. Natl. Acad. Sci. USA, 114, 12685–12690, https://doi.org/10.1073/pnas.1712273114, 2017.