28
Supporting Information Identification of microalgae by laser desorption/ionization mass spectrometry coupled with multiple nanomatrices Lung-Hsiang Peng, a Binesh Unnikrishnan, a Chi-Yu Shih, b Tung-Ming Hsiung, a Jeng Chang, bcd Pang-Hung Hsu, a Tai-Chia Chiu, *e and Chih- Ching Huang *acf a Department of Bioscience and Biotechnology, National Taiwan Ocean University, Keelung, Taiwan; b Institute of Marine Biology, National Taiwan Ocean University, Keelung, Taiwan; c Center of Excellence for the Oceans, National Taiwan Ocean University, Keelung, Taiwan; d Institute of Marine Environmental Chemistry and Ecology, National Taiwan Ocean University, Keelung, Taiwan; e Department of Applied Science, National Taitung University, Taitung, Taiwan; f School of Pharmacy, College of Pharmacy, Kaohsiung Medical University, Kaohsiung, Taiwan S1

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Supporting Information

Identification of microalgae by laser desorption/ionization mass spectrometry coupled with multiple nanomatrices

Lung-Hsiang Peng,a Binesh Unnikrishnan,a Chi-Yu Shih,b Tung-Ming Hsiung,a Jeng Chang,bcd Pang-Hung Hsu,a Tai-Chia Chiu,*e and Chih-Ching Huang*acf

aDepartment of Bioscience and Biotechnology, National Taiwan Ocean University, Keelung, Taiwan; bInstitute of Marine Biology, National Taiwan Ocean University, Keelung, Taiwan; cCenter of Excellence for the Oceans, National Taiwan Ocean University, Keelung, Taiwan; dInstitute of Marine Environmental Chemistry and Ecology, National Taiwan Ocean University, Keelung, Taiwan; eDepartment of Applied Science, National Taitung University, Taitung, Taiwan; fSchool of Pharmacy, College of Pharmacy, Kaohsiung Medical University, Kaohsiung, Taiwan

Correspondence: Tai-Chia Chiu, Department of Applied Science, National Taitung University, 369, Sec. 2, University Rd, Taitung 95092, Taiwan; Tel.: +886-89-517990; Fax: +886-89-518108; E-mail: [email protected]; Chih-Ching Huang, Department of Bioscience and Biotechnology, National Taiwan Ocean University, 2, Pei-Ning Road, Keelung, 20224, Taiwan; Tel.: +886-2-24622192 ext5517; Fax: +886-2-24622320; E-mail: [email protected]

Table S1 List of microalgae strains used in this study.

Taxon

Strain

Order

Family

GenBank Accession no.

Emiliania huxleyi

CCMP373

Isochrysidales

Noelaerhabdaceae

KC404141

Isochrysis galbana

I001

Isochrysidales

Isochrysidaceae

KC888111

Thalassiosira weissflogii

Clone Vic

Thalassiosirales

Thalassiosiraceae

GQ281043

Skeletonema cf. costatum

Kao, Taiwan

Thalassiosirales

Skeletonemaceae

JN676163

Tetraselmis chui

Clone TA

Chlorodendrales

Chlorodendraceae

DQ207405

Nannochloris sp.

CKM

Chlorellales

Chlorellaceae

GQ122381

Table S2 Species-specific peak masses of I. galbana obtained using HgSe, HgTe, HgTeSe, or HgSeHgTeHgTeSe NMs as substrates.

HgSe

HgTe

HgTeSe

HgSeHgTeHgTeSe

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

100.0

55.5

13170.4

100.0

3.3

2315.3

100.0

3.8

7030.6

100.0

105.0

114.9

26091.0

109.0

15.7

10560.8

107.0

3.3

6090.1

105.0

109.0

3.2

703.0

110.0

5.1

3430.9

109.0

4.1

7755.4

107.0

110.0

3.1

677.0

110.3

5.9

3958.0

110.9

6.3

10257.5

109.0

110.3

3.5

768.0

112.0

4.4

2880.8

112.9

3.0

5710.1

110.0

110.9

4.9

1081.0

117.0

4.1

2632.1

114.1

6.5

10511.5

110.3

112.0

5.4

1174.0

119.0

10.5

6803.8

114.9

7.4

11967.5

110.9

114.1

4.9

1086.9

120.0

4.4

2807.5

115.9

4.2

6774.5

112.0

127.0

3.8

789.6

121.0

9.7

6232.5

119.0

3.9

6275.3

112.9

132.0

774.7

156800.3

123.0

3.0

1937.4

121.0

3.0

4916.3

114.1

135.0

296.0

59075.7

123.9

4.7

2971.5

122.9

7.3

11843.8

114.9

137.0

4.1

740.8

126.6

3.4

2128.2

123.9

19.4

37356.5

115.9

139.0

4.2

772.0

127.0

6.6

4145.4

124.9

17.8

34099.2

117.0

146.1

596.0

104265.9

130.0

7.1

4425.1

127.0

22.1

42338.3

119.0

162.1

74.8

11066.1

132.0

192.4

117415.3

132.0

64.9

125885.3

120.0

178.1

12.0

1480.7

135.0

45.0

27322.6

135.0

26.0

50161.8

121.0

179.1

12.4

1530.1

136.0

8.3

4987.2

143.9

5.1

8058.5

122.9

181.7

3.2

374.0

143.0

4.6

2340.5

145.0

7.3

11506.5

123.0

187.1

10.0

1119.1

145.0

7.2

3670.5

146.1

27.6

56579.3

123.9

188.3

7.3

795.6

149.1

7.3

3357.0

149.1

5.5

11308.6

123.9

192.2

12.2

1271.1

151.0

3.3

1739.3

151.0

7.6

15537.9

124.9

206.1

176.1

15837.3

152.0

5.4

2849.9

157.1

4.5

6705.3

126.6

218.1

4.9

378.5

159.1

5.6

2800.2

159.1

4.2

6296.8

127.0

220.1

4.9

377.3

177.1

4.3

1552.0

162.1

6.9

14315.0

130.0

226.0

98.4

7136.3

179.1

3.1

1325.5

165.1

5.1

7666.5

132.0

234.1

114.9

7642.7

187.1

3.5

1172.0

170.9

3.4

7435.3

135.0

250.1

24.2

1263.0

187.7

4.8

1990.4

187.1

4.9

11362.4

136.0

252.2

8180.5

459608.8

192.2

7.3

2462.0

206.1

8.7

20159.0

137.0

252.6

109.1

6130.3

195.3

7.9

8643.0

234.1

4.2

9084.4

139.0

423.0

11.1

452.3

199.2

3.8

1165.3

242.1

3.6

7758.8

143.0

562.4

315.5

10615.5

206.1

9.1

9852.6

246.4

5.8

12042.5

143.9

592.3

6.1

195.2

234.1

14.1

3369.0

252.2

142.5

295657.1

145.0

593.3

31.2

991.4

242.1

3.9

899.5

268.9

4.3

8368.4

146.1

614.3

9.7

291.8

430.4

13.5

2279.0

367.2

3.1

2505.8

149.1

638.3

25.0

721.8

460.2

11.9

1892.0

374.3

20.2

15286.8

151.0

639.2

33.0

950.8

462.3

6.2

990.0

376.0

25.2

18954.5

152.0

660.4

6.2

174.9

533.3

14.3

1964.0

408.0

22.2

15468.5

157.1

666.7

4.4

123.3

562.4

16.7

17348.2

532.2

6.2

3119.3

159.1

672.6

6.5

177.2

592.3

9.3

1085.5

533.3

7.1

3640.0

162.1

700.6

11.3

290.3

593.3

16.0

1855.0

562.4

109.6

51699.2

165.1

726.6

4.0

97.1

614.3

5.0

4986.4

614.3

8.3

3287.2

170.9

770.6

11.6

269.0

700.6

15.4

1240.0

691.0

4.2

1244.2

177.1

772.6

743.3

16919.7

726.6

7.4

505.0

772.6

97.3

13903.2

178.1

786.7

5.5

122.2

772.6

139.9

20509.8

786.7

6.0

808.2

179.1

798.6

16.5

368.0

786.7

8.2

462.0

800.6

137.0

17323.3

181.7

800.6

920.8

20000.1

800.6

174.1

24173.5

820.7

15.7

1732.5

187.1

820.7

4.5

94.9

820.7

12.9

687.0

822.7

5.0

549.6

187.7

822.7

4.5

95.7

826.7

37.0

4815.8

826.7

54.5

5876.3

188.3

826.7

193.5

4083.1

870.6

10.7

1280.3

828.7

18.3

1959.2

192.2

870.6

52.5

1045.8

871.5

11.9

1422.5

870.6

73.5

6104.3

195.3

871.5

83.8

1675.9

872.7

75.5

9022.2

871.5

60.4

5027.2

199.2

872.7

254.8

5070.4

880.7

3.5

414.7

872.7

169.1

14023.5

206.1

879.7

5.6

109.9

877.7

5.7

463.7

218.1

880.7

3.5

69.4

880.7

23.9

1928.5

220.1

881.7

20.8

1678.1

226.0

907.8

9.0

677.4

234.1

909.8

10.4

784.7

242.1

1011.8

5.9

274.3

246.4

250.1

252.2

252.6

268.9

367.2

374.3

376.0

408.0

423.0

430.4

460.2

462.3

532.2

533.3

562.4

592.3

593.3

614.3

638.3

639.2

660.4

666.7

672.6

691.0

700.6

726.6

770.6

772.6

786.7

798.6

800.6

820.7

822.7

826.7

828.7

870.6

871.5

872.7

877.7

879.7

880.7

881.7

907.8

909.8

1011.8

Table S3 Species-specific peak masses of E. huxleyi obtained using HgSe, HgTe, HgTeSe, or HgSeHgTeHgTeSe NMs as substrates.

HgSe

HgTe

HgTeSe

HgSeHgTeHgTeSe

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

100.0

140.4

45468.2

100.0

42.0

20938.0

100.0

20.5

6686.2

100.0

102.9

7.1

1974.8

107.0

10.2

4999.4

102.9

5.8

1871.4

102.9

105.0

23.1

6456.5

109.0

18.0

8833.8

107.0

8.9

2903.5

105.0

107.0

5.0

1406.5

110.3

5.6

2700.8

109.0

18.6

6088.3

107.0

109.0

5.1

1412.5

112.0

3.7

1768.3

110.3

5.7

1833.3

109.0

110.3

7.5

2058.5

112.3

5.7

2732.6

112.0

5.8

1857.1

110.3

110.9

8.0

2194.5

114.1

7.3

3478.9

114.1

4.2

1317.5

110.9

112.0

4.7

1286.5

117.0

8.7

4166.9

114.4

3.6

1120.5

112.0

114.1

23.1

7533.2

118.0

11.3

5394.7

116.0

4.1

1262.5

112.3

117.0

7.6

2468.7

119.0

9.9

4673.9

117.0

6.8

2097.5

114.1

118.0

19.7

6345.4

121.0

27.4

12908.5

118.0

18.5

5862.6

114.4

119.0

3.9

1263.7

123.0

5.2

2481.9

119.0

8.7

2747.9

116.0

120.0

3.2

872.3

132.0

86.5

40206.0

121.0

39.5

12539.1

117.0

121.0

33.2

10892.7

135.0

11.0

5050.3

123.0

4.3

1338.7

118.0

126.1

3.5

1123.9

143.0

3.9

1574.0

132.0

108.1

33748.4

119.0

132.0

136

45087.5

145.1

5.4

2406.5

135.0

8.9

2717.9

120.0

134.0

9.3

3006.7

159.1

4.5

1875.4

144.0

3.2

914.1

121.0

136.0

3.1

983.5

184.0

105.6

38373.0

145.1

3.4

1008.2

123.0

139.0

9.0

2887.9

549.2

18.7

3017.0

149.0

7.8

2292.3

126.1

140.0

7.7

2487.6

593.3

16.1

2338.5

158.1

10.4

2983.9

132.0

145.1

10.1

3212.4

608.2

8.5

1189.0

159.1

4.5

1280.0

134.0

147.0

5.4

1708.5

614.2

3.6

3187.2

184.0

122.6

32984.7

135.0

149.0

3.1

990.8

700.6

4.9

501.5

201.0

7.2

1499.5

136.0

154.1

6.5

2049.7

870.6

4.6

275.5

203.2

11

6120.8

139.0

161.1

3.2

989.8

871.6

5.6

340.4

228.3

78.3

43062.4

140.0

162.1

7.1

2183.3

872.6

12.9

775.9

252.1

24.2

13070.4

143.0

169.0

3.7

1118.9

284.3

4.2

2188.3

144.0

181.7

4.6

1332.4

303.6

3.2

1627.3

145.1

184.0

160.4

46202.3

402.4

4.9

632.0

147.0

226.1

6.4

946.5

494.6

14.4

4052.5

149.0

247.2

6.8

1478.8

522.6

30.4

8527.2

154.1

252.1

130.4

25934.4

549.2

24.1

10485.9

158.1

298.8

3.2

460.6

614.2

6.1

2615.9

159.1

398.2

3.7

291.1

660.4

7.3

691.0

161.1

434.9

6.0

443.9

672.6

9.8

883.0

162.1

456.9

4.5

314.7

870.6

12.9

629.3

169.0

593.3

4.0

209.0

871.6

10.6

515.0

181.7

614.2

13.3

656.8

872.6

15.0

731.6

184.0

867.6

3.7

106.8

1316.2

8.4

177.2

201.0

1318.1

12.1

257.0

203.2

1364.2

3.1

62.0

226.1

228.3

247.2

252.1

284.3

298.8

303.6

398.2

402.4

434.9

456.9

494.6

522.6

549.2

593.3

608.2

614.2

660.4

672.6

700.6

867.6

870.6

871.6

872.6

1316.2

1318.1

1364.2

Table S4 Species-specific peak masses of T. weissflogii obtained using HgSe, HgTe, HgTeSe, or HgSeHgTeHgTeSe NMs as substrates.

HgSe

HgTe

HgTeSe

HgSeHgTeHgTeSe

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

102.0

5.6

886.1

100.2

6.0

576.9

102.0

5.7

2222.7

100.2

110.0

11.8

1759.9

101.0

3.4

329.0

113.6

13.9

5055.9

101.0

113.6

26.6

3839.4

102.0

5.0

479.6

117.0

4.2

1501.6

102.0

118.0

4.3

614.6

109.1

32.2

2971.8

130.0

13.1

4481.5

109.1

120.0

7.5

1049.2

110.0

21.8

1988.0

132.1

389.6

131292.4

110.0

132.1

940.9

118848.3

110.3

18.8

1711.5

136.0

9.9

3309.3

110.3

134.9

4.4

546.0

112.3

32.7

2957.5

152.1

5.6

1715.7

112.3

136.0

5.4

662.4

113.6

39.7

3581.5

178.1

9.5

2425.3

113.4

140.0

12.1

1282.0

113.4

21.2

1917.5

184.1

170.2

41750.0

113.6

140.3

18.4

1959.0

117.0

3.6

317.6

218.1

9.3

2775.5

117.0

142.1

5.1

545.0

118.0

8.1

723.8

252.1

97.0

26554.4

118.0

178.1

22.0

1716.5

119.0

17.2

1577.1

365.1

32.5

3538.8

119.0

184.1

568.2

39224.3

120.0

22.5

2038.1

394.4

3.1

342.4

120.0

198.1

3.0

175.2

121.1

10.9

949.0

396.4

3.9

441.4

121.1

218.1

34.9

1796.7

125.1

9.6

819.8

444.3

5.2

632.0

125.1

226.1

8.7

419.5

125.9

3.7

316.7

459.2

29.8

3658.6

125.9

252.1

284.5

12811.1

127.1

10.0

858.2

460.2

13.7

1674.6

127.1

276.1

4.4

200.0

127.9

16.2

1445.5

461.3

8.5

1041.6

127.9

308.3

3.4

155.7

130.0

22.8

1923.8

467.2

4.1

505.0

130.0

365.1

7.0

343.4

132.1

1285.6

107316.6

472.3

4.4

546.6

132.1

459.2

11.9

597.0

134.9

4.8

392.4

481.2

10.5

1562.0

134.9

472.3

3.3

163.3

136.0

15.5

1273.9

490.3

23.5

2941.4

136.0

484.0

4.9

226.2

138.7

4.7

373.2

506.0

23.7

2760.0

138.7

490.3

11.9

596.9

139.1

6.6

531.4

518.3

6.4

806.0

139.1

506.0

10.7

495.1

145.1

6.9

533.9

519.2

19.3

2430.0

140.0

519.2

8.1

407.4

147.1

13.7

1037.0

527.1

36.3

4581.4

140.3

527.1

9.9

500.5

149.1

7.0

513.2

533.2

22.7

3296.1

142.1

533.2

8.3

421.3

178.1

16.8

1031.7

536.4

6.7

972.5

145.1

592.2

6.7

336.1

184.1

519.1

28957.3

549.3

3.0

444.6

147.1

593.2

8.8

440.8

218.1

14.6

688.1

562.3

3.5

515.6

149.1

614.1

14.8

740.5

225.2

3.8

169.6

591.4

5.8

854.5

152.1

638.1

8.7

468.5

252.1

154.3

6513.2

592.2

14.5

2138.0

178.1

639.0

10.4

556.5

282.3

3.4

142.0

593.2

17.6

2589.4

184.1

672.4

11.3

617.0

308.3

6.9

299.9

614.1

28.8

4213.7

198.1

698.4

36.8

2039.5

339.3

3.7

161.5

672.4

12.2

1858.0

218.1

700.4

43.9

2444.9

365.1

20.3

921.9

689.2

7.9

1233.3

225.2

712.4

3.0

166.4

445.2

13.1

600.5

698.4

23.4

3760.3

226.1

722.4

13.3

747.4

459.2

22.2

1017.5

700.4

27.9

4500.1

252.1

724.4

78.6

4421.7

460.2

11.5

527.4

722.4

10.2

1683.8

276.1

726.4

140.4

7842.8

467.2

4.9

224.6

724.4

42.4

7009.7

282.3

728.5

7.8

435.6

481.2

12.1

545.9

726.4

67.5

11033.9

308.3

738.4

6.1

341.7

484.0

7.1

303.0

736.5

3.3

528.9

339.3

746.4

87.4

4910.8

490.3

17.7

804.4

738.4

6.3

1001.9

365.1

748.4

34.7

1940.3

506.0

32.5

1418.2

746.4

48.9

7748.9

394.4

750.4

53.5

2979.6

507.6

14.9

670.9

748.4

22.0

3455.9

396.4

752.4

142.6

7935.3

509.5

12.9

581.5

750.4

33.4

5210.6

444.3

754.5

123.9

6835.1

511.5

18.6

842.3

752.4

67.2

10418.0

445.2

760.4

6.3

341.2

513.5

14.7

659.9

754.5

60.8

9380.7

459.2

762.4

3.4

182.5

515.6

7.3

327.1

772.4

135.6

16530.5

460.2

770.4

13.8

620.0

518.3

3.4

152.5

774.4

157.9

19073.0

461.3

772.4

236.2

12497.2

519.2

14.7

662.8

776.5

41.2

4958.1

467.2

774.4

283.5

14936.3

527.1

26.4

1193.2

778.6

15.9

1913.0

472.3

776.5

66.8

3502.6

533.2

22.9

1032.2

780.5

7.1

851.4

481.2

780.5

11.8

613.9

562.3

4.3

193.5

786.5

7.9

919.7

484.0

786.5

10.4

533.6

571.2

6.3

282.7

788.5

4.3

500.7

490.3

788.5

4.6

237.2

592.2

16.3

726.1

794.5

4.3

488.8

506.0

794.5

4.7

239.7

593.2

12.9

577.8

796.5

13.2

1491.4

507.6

796.5

17.8

900.8

614.1

63.4

2798.0

798.4

96.5

10861.2

509.5

798.4

148.6

7485.4

660.3

3.3

141.5

800.4

216.8

24261.1

511.5

800.4

388.8

19559.1

672.4

12.3

540.2

814.5

3.7

394.0

513.5

814.5

4.1

201.0

698.4

32.0

1403.2

820.4

41.7

4406.6

515.6

820.4

56.0

2697.4

700.4

44.2

1952.5

822.5

26.2

2756.2

518.3

822.5

33.5

1606.2

722.4

9.6

420.6

824.5

18.9

1977.6

519.2

824.5

24.7

1177.2

724.4

74.8

3266.7

826.5

10.0

1035.2

527.1

826.5

12.6

598.9

726.4

135.4

5860.1

846.4

122.5

12302.5

533.2

846.4

177.4

8083.3

746.4

98.3

4095.7

851.2

3.7

352.2

536.4

870.4

22.3

956.3

748.4

35.9

1486.4

870.4

37.6

3500.0

549.3

871.4

22.6

970.9

750.4

52.0

2150.9

871.4

35.3

3281.9

562.3

752.4

147.4

6109.4

966.9

11.2

428.0

571.2

754.5

126.8

5215.9

968.9

18.3

703.0

591.4

772.4

241.0

9504.1

981.0

6.2

219.0

592.2

774.4

325.3

12780.6

983.0

8.4

296.0

593.2

776.5

69.8

2724.7

614.1

780.5

9.6

373.2

638.1

786.5

7.4

280.3

639.0

788.5

3.5

132.1

660.3

794.5

4.2

157.4

672.4

796.5

13.4

495.4

689.2

798.4

154.2

5711.1

698.4

800.4

451.5

16607.7

700.4

820.4

74.7

2626.5

712.4

822.5

42.9

1505.7

722.4

824.5

26.5

925.3

724.4

826.5

10.4

362.4

726.4

836.5

3.4

116.9

728.5

846.4

229.4

7774.4

736.5

870.4

57.4

1825.1

738.4

871.4

34.6

1097.1

746.4

966.9

4.8

111.5

748.4

968.9

10.8

248.1

750.4

752.4

754.5

760.4

762.4

770.4

772.4

774.4

776.5

778.6

780.5

786.5

788.5

794.5

796.5

798.4

800.4

814.5

820.4

822.5

824.5

826.5

836.5

846.4

851.2

870.4

871.4

966.9

968.9

981.0

983.0

Table S5 Species-specific peak masses of Nannochloris sp. obtained using HgSe, HgTe, HgTeSe, or HgSeHgTeHgTeSe NMs as substrates.

HgSe

HgTe

HgTeSe

HgSeHgTeHgTeSe

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

118.0

5.9

228.8

102.0

15.9

5873.6

102.0

34.8

4403.3

102.0

128.0

5.9

219.0

138.0

3.7

1257.5

118.0

5.5

667.2

118.0

138.0

11.2

407.8

168.1

4.4

1405.3

138.0

10.1

1202.6

128.0

140.0

4

146.5

170.1

8.0

2552.3

170.1

3.0

371.0

138.0

170.1

4.9

146.5

184.0

27.1

8381.4

184.0

28.5

3610.3

140.0

175.1

25.2

757.9

230.1

5.6

1258.0

269.0

14.1

1114.0

168.1

184.0

171

4948.4

269.0

6.1

1244.0

319.9

15.5

1165.0

170.1

203.9

3.9

97.7

365.2

14.0

2495.0

614.2

28.1

1828.3

175.1

614.2

6.5

100.9

614.2

3.2

3917.2

660.4

13.0

785.0

184.0

660.4

6.6

96.5

660.4

4.9

563.0

203.9

230.1

269.0

319.9

365.2

614.2

660.4

Table S6 Species-specific peak masses of S. cf. costatum obtained using HgSe, HgTe, HgTeSe, or HgSeHgTeHgTeSe NMs as substrates.

HgSe

HgTe

HgTeSe

HgSeHgTeHgTeSe

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

101.0

3.7

122.6

100.0

10.6

240.5

101.0

8.3

1662.4

100.0

102.0

4.7

154.7

101.0

7.3

167.3

102.0

12.5

2495.7

101.0

110.0

64.5

2079.6

102.0

13.7

313.9

120.0

58.4

10944.0

102.0

112.0

79.3

2555.5

107.0

3.2

71.4

129.1

27.9

4986.2

107.0

113.1

25.6

815.0

110.0

61.0

1354.4

130.0

35.8

6344.7

110.0

120.0

56.8

1893.5

120.0

103.6

2270.0

132.1

26.4

4644.6

112.0

125.1

4.5

138.7

125.1

20.8

454.0

134.0

3.9

687.7

113.1

127.1

5.0

154.2

127.9

70.6

1567.9

136.0

71.0

12385.6

120.0

129.1

74.5

2275.5

129.9

81.2

1791.1

152.0

54.6

8453.3

125.1

132.1

18.4

569.1

130.0

79.9

1708.9

184.1

279.4

33109.1

127.1

133.0

7.6

230.5

132.1

23.8

514.1

252.2

43.7

3301.6

127.9

136.0

31.0

947.3

136.0

54.7

1142.6

252.8

74.5

5574.8

129.1

141.1

4.1

117.6

146.1

6.2

131.0

591.4

3.1

212.3

129.9

146.1

7.2

208.7

147.0

3.7

75.0

592.3

4.0

276.2

130.0

147.0

4.1

117.7

152.0

13.4

268.2

593.4

6.1

426.1

132.1

152.0

7.2

200.7

154.1

24.1

489.6

133.0

154.1

46.8

1285.6

159.1

4.6

92.5

134.0

184.1

648.5

15922.0

162.1

4.6

90.1

136.0

215.0

81.8

1825.8

184.1

603.0

11166.3

141.1

252.2

16.9

362.7

186.1

58.9

1096.0

146.1

252.2

14.5

244.8

147.0

308.3

25.2

422.8

152.0

154.1

159.1

162.1

184.1

186.1

215.0

252.2

252.8

308.3

591.4

592.3

593.4

Table S7 Species-specific peak masses of T. chui obtained using HgSe, HgTe, HgTeSe, or HgSeHgTeHgTeSe NMs as substrates.

HgSe

HgTe

HgTeSe

HgSeHgTeHgTeSe

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

S/N

Intens.

m/z

100.0

13.1

2069.8

100.0

14.3

2003.9

110.2

17.8

12900.7

100.0

101.0

3.2

513.8

101.0

7.0

975.5

125.9

4.8

3271.7

101.0

102.0

4.8

754.5

102.0

14.0

1974.0

127.0

5.4

3660.3

102.0

110.2

39.2

6036.5

107.0

6.3

864.2

129.1

7.2

4903.9

107.0

112.0

24.1

3706.0

110.2

101.2

13409.0

130.0

17.7

12017.4

110.2

120.0

15.5

2327.5

112.0

43.5

5825.7

131.1

4.6

3060.2

112.0

125.0

20.0

2864.6

114.0

7.7

1016.8

133.1

4.7

3150.6

114.0

127.0

3.0

431.7

116.0

10.6

1447.4

134.9

11.3

7509.7

116.0

130.0

8.5

1208.8

118.0

4.0

517.0

136.0

38.0

25321.5

118.0

134.9

20.0

2679.8

119.0

4.8

620.2

138.1

9.8

6442.9

119.0

136.0

31.8

4231.7

120.0

31.6

4151.6

152.0

23.1

13881.4

120.0

138.1

3.3

441.6

121.1

6.5

843.1

159.1

10.3

5800.9

121.1

147.0

11.8

1487.5

125.0

5.3

666.7

160.1

3.8

2120.2

125.0

152.0

9.9

1176.9

125.9

7.0

884.9

166.1

8.0

4233.3

125.9

157.2

4.9

555.2

127.0

6.9

873.1

184.1

481.6

209083.3

127.0

166.1

15.1

1629.7

127.9

16.7

2165.7

198.1

10.5

4495.4

127.9

175.1

107.3

10754.8

129.1

12.9

1608.4

199.2

37.5

16074.6

129.1

184.1

1103.1

102470.5

129.9

19.8

2585.7

202.2

3.0

1239.9

129.9

199.2

31.5

2745.3

130.0

36.1

4532.0

206.1

4.7

1919.1

130.0

236.2

7.7

551.2

134.9

15.7

1877.9

207.1

3.1

1275.3

131.1

308.3

4.1

255.9

136.0

71.6

8673.9

236.2

7.3

2412.1

133.1

467.1

6.2

425.9

138.1

6.1

717.9

268.1

5.6

1350.0

134.9

481.1

16.5

1143.0

148.0

23.7

2646.3

281.1

6.6

1735.6

136.0

505.5

30.1

2023.5

152.0

24.9

2588.4

459.3

5.9

1713.8

138.1

614.1

4.4

270.5

157.2

4.5

445.5

460.3

3.8

1080.6

147.0

704.5

6.8

357.0

159.1

14.9

1441.0

467.1

9.4

2691.8

148.0

734.5

3.4

171.9

160.1

5.6

551.7

468.2

3.8

1079.7

152.0

758.5

6.4

311.0

166.1

11.6

1064.5

481.1

18.5

5130.7

157.2

175.1

264.9

22755.2

483.4

4.9

1279.5

159.1

184.1

1474.4

117038.0

495.1

4.5

1226.7

160.1

198.1

9.1

683.8

497.1

4.2

1147.6

166.1

206.1

5.7

406.3

505.5

28.6

7448.6

175.1

236.2

10.6

618.0

533.2

3.1

965.5

184.1

467.1

24.2

1769.0

571.2

3.4

1025.1

198.1

481.1

52.5

3833.8

614.1

8.4

2349.9

199.2

495.1

6.7

488.3

704.5

32.0

6445.8

202.2

497.1

6.1

443.6

706.6

4.6

919.9

206.1

505.5

80.6

5621.9

732.6

5.1

959.0

207.1

519.7

8.6

571.6

734.5

19.5

3686.0

236.2

533.2

3.0

231.3

736.6

13.0

2440.8

268.1

555.2

4.4

325.9

758.5

29.6

5303.3

281.1

571.2

7.4

532.9

760.5

13.2

2354.3

308.3

593.2

3.1

243.3

780.6

8.8

666.8

459.3

614.1

19.0

1500.3

782.5

17.9

1350.8

460.3

704.5

14.8

1134.8

784.5

34.2

2577.0

467.1

734.5

5.9

440.6

786.6

6.1

455.8

468.2

736.6

4.8

354.0

804.5

39.2

2758.8

481.1

758.5

9.9

712.5

806.5

43.7

3076.4

483.4

760.5

5.2

375.8

808.6

6.8

473.2

495.1

782.5

4.2

272.6

870.5

8.7

489.9

497.1

784.5

8.8

577.1

871.6

9.5

534.8

505.5

804.5

9.9

637.3

519.7

806.5

11.9

771.7

533.2

555.2

571.2

593.2

614.1

704.5

706.6

732.6

734.5

736.6

758.5

760.5

780.6

782.5

784.5

786.6

804.5

806.5

808.6

870.5

871.6

Table S8 Reproducibility of the LDI-MS analysis of the six microalgae by the three HgSe, HgTe, and HgTeSe nanomatrices from five repetitive measurements.

Algae

Nanomatrices

No. of significant peaks

(fed to Venn diagram construction)

Average RSD (%)

I. galbana

HgSe

54

9.1

HgTe

52

11

HgTeSe

58

9.2

E. huxleyi

HgSe

39

20

HgTe

26

10.2

HgTeSe

42

5.1

T. weissflogii

HgSe

68

8.8

HgTe

90

4.0

HgTeSe

72

13.7

Nannochloris sp.

HgSe

10

9.8

HgTe

10

12.9

HgTeSe

9

10.9

S. cf. costatum

HgSe

20

17.3

HgTe

22

14.3

HgTeSe

15

17.0

T. chui

HgSe

28

5.8

HgTe

54

9.1

HgTeSe

51

9.7

Fig. S1 EDS spectra of prepared (a) HgSe, (b) HgTe, and (c) HgTeSe NMs.

Fig. S2 STEM-EDS elemental mapping of the prepared (a) HgSe, (b) HgTe, and (c) HgTeSe NMs.

Fig. S3 UV-vis absorption spectra of the prepared HgTe, HgSe, and HgTeSe NMs (0.025X) in DI water. Absorbance (Abs) is plotted in arbitrary units (a. u.).

Fig. S4 XRD spectra of (a) HgSe, (b) HgTe, and (c) HgTeSe NMs.

Fig. S5 Light microscope (400X) images of the tested microalgae; (a) I. galbana, (b) E. huxleyi, (c) T. weissflogii, (d) Nannochloris sp, (e) S. cf. costatum, and (f) T. chui.

Fig. S6 Background mass spectra recorded using (a) HgSe NMs, (b) HgTe NMs, (c) HgTeSe NMs, (d) DHB, (e) HCCA, and (f) SA as matrices. Other conditions were the same as those described in Fig. 1

S2