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Design and Applications of Luminescent Logic Systems. Molecular Logic Gates Nimal Gunaratne, Colin McCoy Nature 1993, 364 , 42. generalization. integration. numeracy. games. reconfiguring. George Boole 1849-64, Cork. improved sensing. object identification.

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Design and Applications of

Luminescent Logic Systems


Molecular

Logic Gates

Nimal Gunaratne, Colin McCoy

Nature 1993, 364, 42

generalization

integration

numeracy

games

reconfiguring

George Boole

1849-64, Cork

improved sensing

object identification


Miyashita

Kim, Yoon,

James, Stoddart, Parker, Beer, Chin, Grigg,

Williams, Tucker, Zauner, Fallis, Aldridge

Andreasson, Sun

Choi, Zhang

Iwai, Okamoto,

Schneider, Rurack,

Wu

Sugimoto, Hirai,

Voegtle, Schmittel,

Steer, Yeow,

Tomizaki, Matsui,

Benenson, Walt

Ihmels, Theato

Yuan, Fang,

Leigh,

Wettig

Callan,

Fujimoto, Akashi,

Zhang, Zhu,

Callan

de Silva

Miyashita, Hamachi

Yan, Li, Fu,

de Silva,

Yurke

Redmond,

Shi, Tong,

Uchiyama, Aida,

Szacilowski,

Gunnlaugsson,

MacDonaill

Wang, Xing,

Tanaka, Fujita,

Samoc

Konermann

Vasquez-

Wu, Shi

Mihara, Nojima,

Remacle

Wasielewski,

Lopez

Kinbara

Lehn

Lu

Conrad, Liu, Smith

Pina, Pischel

Birge,

Stojanovic,

Seeman,

Avouris,

Katz, Privman,

Sokolov, Wang

Kimura,

Levine, Speiser,

Shanzer,

Willner,

Shabat,

Ashkenasy,

Lotan,

Van der Boom,

Rabani,

Shapiro,

Eichen

Jin

Bazan

Perez-

Stoddart,

Heath, Smolke

Kubo

Inestrosa,

Tian, Wang, Jin,

Liu

Pischel

Huang, Zhang, Yu,

Adleman,

Ghadiri,

Qian, He

Reif

Garcia-

Espana,

Chiu

Lerner,

Miranda,

Barbas,

Raymo, Zhu,

Bharadwaj, Khan,

Covera

Kolpashnikov,

Wang

Upadhyay

Johnson

Lu, Ma

Samanta

Breaker,

Yang

Hamilton

Brown

Ji

Toma

Gust, Moore

Akkaya

Bouas-Laurent, Desvergne,

Bassani, McClenaghan

Das

Balzani, Credi,

Venturi, Gentili,

Langford,

Stefanovic,

Doorn

Evans

Kumar,

Diederich, Constable, Schluter

Pallavicini, Fabbrizzi,

Bhalla,

Campagna, Quici

Singh


Dong, Ren,

Alexander, Jones, Steed

Stokke

Kong,

Wang, Qu,

Zhu

Jiang

Mayer, Nau, Schalley,

Seeberger, Schiller

Jang

Budyka

Stoddart

Ha, Lee, Kim, Oh

Flood

Wang, Jiang, Hu

deSouter-Lecomte

Magri

Suzuki, Araki

Shvarev

Jia

Pita

Hill, Ariga

Alfonta

Zhang

Zink,

Dwyer

Yamada, Ogawa,

Plaxco

Siri

Pandey

Maeda

Ruiz-Molina

Nandi

Cheng

Pasparakis

D’Souza

Jiang

Sessler, Tour

Zhang, Ye,

Leung

Darwish,

Hanley

Huang

Tuntulani

Humphrey

Ajayaghosh

Kandaswamy


IN

IN

IN1

IN2

OUT

OUT

OUT

YES

NOT

AND

IN1

IN2

OUT

IN

OUT

OUT

0

0

1

0

0

0

1

0

1

0

1

0

1

0

0

1

1

1


Luminescent molecular switchable systems can gather and process information

Digital 1

Analog region

Optical

response

Digital 0

Chemical stimulus level


Molecular Computation in a Small Nanospace process information

Seiichi Uchiyama, Gareth McClean,

Kaoru Iwai (Nara Women’s University)

J. Am. Chem. Soc. 2005, 127, 8920


3 nm process information

Soap micelle

with ion cloud


receptor process information

receptor

receptor

receptor

1

1

2

2

fluorophore

fluorophore

anchor

anchor

spacer

spacer

spacer

spacer

+

+

H

H

Na

Na

O

O

O

N

O

O

O

O

S

N

3


and process information

+

+

H

H

H

H

+

+

Na

Na

IF

none

0

400

400

500

500

Wavelength (nm)


Combining Several Diagnostic Tests and Data Processing process information

in a

“Lab-on-a-Molecule”

David Magri, Gareth McClean, Gareth Brown

J. Am. Chem. Soc. 2006, 128, 4950


Full Blood Count process information

Date : 20.08.2005

Description Result Units Reference Ranges Remarks

Haemoglobin 8.70* g/dl 12.00 17.50 Low

RBC 2.34* x 10x6/mm3 3.50 6.00 Low

PCV 26.70* % 40.00 54.00 Low

MCV 114.10* fl 70.00 96.00 High

MCH 37.20 pg 27.00 32.00 High

MCHC 32.60 g/dl 30.00 ….35.00 …Normal

PLATELETS 140,000.00 mm3 150,000.00 450,000.00 Low

WBC 8,200.00 mm3 4,000.00 11,000.00 Normal

NEUTROPHILS 48.00 % 40.00 75.00 …normal

LYMPHOCYTES48.00 % 10.00 45.00 High

EOSINOPHILS 2.0 % 1.00 6.00 Normal

MONOCYTES 2.00 % < 10.00 Normal

Performed by Sysmex/Hycell Automated Haematology Analyzers

Logical combination of ‘high’ and ‘low’

parameters identifies disease


Spacer process information

Receptor

Spacer

Receptor

Receptor

+

+

Na

H

H

2+

Zn

O

-

O

C

O

2

O

-

N

C

O

N

O

2

O

Spacer

Fluorophore


+ process information

+

2+

Na

, H

, Zn

+

+

Na

, H

+

2+

Na

, Zn

+

Na

IF

+

2+

H

, Zn

2+

Zn

+

H

No inputs

0

400

440

480

520

Wavelength / nm


3-Input AND Logic Truth Table process information

Input1

Na+

Input2

H+

Input3

Zn2+

Output FluornF

0 (low)

0 (low)

0 (low)

0 (low, 0.001)

0 (low)

1 (high)

0 (low)

0 (low, 0.001)

0 (low)

0 (low)

1 (high)

0 (low, 0.002)

0 (low)

1 (high)

1 (high)

0 (low, 0.003)

1 (high)

0 (low)

0 (low)

0 (low, 0.006)

1 (high)

1 (high)

0 (low)

0 (low, 0.007)

1 (high)

0 (low)

1 (high)

0 (low, 0.006)

1 (high)

1 (high)

1 (high)

1 (high, 0.020)


Molecular Computational process information

Identification (MCID)

of Small ObjectsinPopulations

Sheenagh Weir,Bernie McKinney

Dave Pears, Mark James (Avecia)

Nature Mater. 2006, 5, 787


Radiofrequency Identification (RFID): process information

The semiconductor technology approach to identifying each object (Goods, People) in an entire population

1 mm x 1 mm RFID chip (Hitachi)


Prefabricated process information YES logic gate fixed to

polymer bead (0.1 mm)

422

100

Increasing pH

401

446

Fluorescence Intensity

0

Wavelength (nm)

500

385

EXCITATION WAVELENGTH:368 nm


Prefabricated logic gates fixed to polymer beads process information

NOT

PASS 1

YES

O

N

O

N

H

N

H

100

PASS 1

I

YES

F

NOT

0

1

3

5

7

9

11

pH


Arraying gates with identical fluorophores process information

and different logic type

2.5 % loading

2.5 % loading

H

H

N

N

422

N

100

O

O

Increasing pH

446

401

I

F

0

385

500

Wavelength (nm)


Input process information

(H+)

Output

(Fluorescence)

Output

(Fluorescence)

Total Output

(Fluorescence)

0

1

0

1

100

80

1

1

1

2

60

Emission (at 422 nm)

40

20

0

2.5

4.5

6.5

8.5

10.5

OUT

( Blue fluorescence)

pH

IN

(H+)

OUT

( Blue fluorescence)

pKa : 4.4


Multi-valued logic is available for process information

molecular computational identification

c.f. binary logic needed in semiconductor computing

Combinations of:

Many (>5) excitation colours

Many (>5)emission colours

Many (>5) types (YES, NOT, PASS 1, AND,…)

Many (>5)chemical inputs (H+, Na+,…)

Many (>2)thresholds (pH 7, pH 4,…)

Many(>5)combinations (YES + PASS 1, YES + 2 PASS 1,…)

Conservatively, millions of mm objects can be encoded!


A process information

D

C

B

A; PASS 1

B; NOT

C; PASS 1

D; PASS 1 + YES (1:1)

E; YES

F; NOT

G; PASS 1

I; YES

J; PASS 0

acid

E

G

F

I

J

A

D

B

C

alkali

E

G

F

I

J


“Plug-and-Play” Logic via Self-Assembly process information

Vinny Vance, Catherine Dobbin,

Boontana Wannalerse

Chem. Commun. 2009, 1386


Covalently bound YES Logic: process information

n

-

C

H

9

1

9

N

N

Self-Assembled YES Logic:

L

II

Ru

N

N

Assembler: Non-ionic Detergent Micelle

n

-

C

H

S

9

1

9

2

-

O

L

R

R

O

H

O

10

Long-lived (100 ns) lumophore


- process information

O

pKa = 9.9


Covalently bound AND Logic: process information

-

-

C

O

C

O

L

2

2

N

O

n

-

C

H

8

1

7

Self-Assembled AND Logic:

S

S

-

O

L

R1

R1

R2

R2

Log bCa2+ = 1.5

pKa = 9.9

pKa = 5.8


- process information

O

-

-

11; 10-8 M H+ and 0.2 M Ca2+

C

O

C

O

2

2

01; 10-12 M H+ and 0.2 M Ca2+

N

10; 10-8 M H+ only

O

00; 10-12 M H+ only

n

-

C

H

8

1

7


Covalently bound OR Logic: process information

-

-

C

O

C

O

2

2

Non-selective Receptor

N

L

O

n

-

C

H

8

1

7

Self-Assembled OR Logic:

S

binds H+ or Ca2+

L

R

R

pKa = 5.8

Log bCa2+ = 1.5


- process information

-

11; 10-4 M H+ and 0.2 M Ca2+

C

O

C

O

2

2

10; 10-4 M H+ only

N

01; 10-8 M H+ and 0.2 M Ca2+

O

00; 10-8 M H+ only

n

-

C

H

8

1

7


Logic Gates with process information

Temperature Input

Seiichi Uchiyama, Narumi Kawai

Kaoru Iwai (Nara Women’s University)

J. Am. Chem. Soc. 2004, 126, 3032


O process information

O

and

Temperature-sensitive co-polymer

N

H

N

H

N

M

e

2

O

O

Co-polymerizable polarity sensor

(Emission weakens in water)

N

N

O

N

S

O

N

M

e

2

2


pH 7 process information

IF

0

10

20

30

40

Temperature / C


pH 9 process information

IF

pH 8

pH 7

pH 5

0

60

20

40

0

80

Temperature / C


2-Input INHIBIT Logic Truth Table process information

Input1

Temperature

Input2

H+

Output

Fluorescence

0 (low; 10 C)

0 (low; 10-9 M)

0 (low; 1)

0 (low; 10 C)

0 (low; 1)

1 (high; 10-5 M)

1 (high; 35 C)

0 (low; 10-9 M)

1 (high; 10)

1 (high; 35 C)

1 (high; 10-5 M)

0 (low; 1)


EPSRC process information

DENI

EUROPEAN COMMISSION

JAPAN SOCIETY FOR

THE PROMOTION OF SCIENCE

Providence

Luck

Serendipity


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