Nonlinear spectroscopy with quantum entangled photons is an emerging field of research that holds the promise to achieve superior signal-to-noise ratio and effectively isolate many-body interactions. Photon sources used for this purpose, however, lack the frequency tunability and spectral bandwidth demanded by contemporary molecular materials. Here, we present design strategies for efficient spontaneous parametric downconversion to generate biphoton states with adequate spectral bandwidth and at visible wavelengths. Importantly, we demonstrate, by suitable design of the nonlinear optical interaction, the scope to engineer the degree of spectral correlations between the photons of the pair. We also present an experimental methodology to effectively characterize such spectral correlations. Importantly, we believe that such a characterization tool can be effectively adapted as a spectroscopy platform to optically probe system–bath interactions in materials.
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28 August 2023
Research Article|
August 24 2023
Measurement principles for quantum spectroscopy of molecular materials with entangled photons
Special Collection:
JCP and CPR Editors’ Choice 2024
,
2023 JCP Emerging Investigators Special Collection
Luca Moretti
;
Luca Moretti
(Data curation, Formal analysis, Investigation, Software, Writing – original draft)
1
Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
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Esteban Rojas-Gatjens
;
Esteban Rojas-Gatjens
(Data curation, Formal analysis, Investigation, Software, Visualization, Writing – original draft)
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
3
School of Chemistry and Biochemistry, Georgia Institute of Technology
, Atlanta, Georgia 30332, USA
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Lorenzo Uboldi
;
Lorenzo Uboldi
(Data curation, Formal analysis, Investigation, Visualization, Writing – review & editing)
1
Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
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David Otto Tiede
;
David Otto Tiede
(Data curation, Formal analysis, Investigation, Writing – review & editing)
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
4
Institute of Materials Science of Sevilla, Spanish National Research Council
, Américo Vespucio, 49, 41092 Sevilla, Spain
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Evan J. Kumar
;
Evan J. Kumar
(Data curation, Investigation, Visualization)
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
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Chiara Trovatello
;
Chiara Trovatello
(Investigation, Resources, Writing – review & editing)
1
Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
5
Department of Mechanical Engineering, Columbia University
, New York, New York 10027, USA
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Fabrizio Preda
;
Fabrizio Preda
(Resources)
6
NIREOS S.R.L.
, Via G. Durando 39, 20158 Milano, Italy
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Antonio Perri
;
Antonio Perri
(Resources)
6
NIREOS S.R.L.
, Via G. Durando 39, 20158 Milano, Italy
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Cristian Manzoni
;
Cristian Manzoni
(Conceptualization, Formal analysis, Methodology, Writing – review & editing)
7
IFN-CNR, Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
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Giulio Cerullo
;
Giulio Cerullo
(Conceptualization, Funding acquisition, Project administration, Supervision, Writing – original draft)
1
Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
7
IFN-CNR, Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
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Ajay Ram Srimath Kandada
Ajay Ram Srimath Kandada
a)
(Conceptualization, Funding acquisition, Project administration, Supervision, Writing – original draft)
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
a)Author to whom correspondence should be addressed: [email protected]
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Luca Moretti
1,2
Esteban Rojas-Gatjens
2,3
Lorenzo Uboldi
1,2
David Otto Tiede
2,4
Evan J. Kumar
2
Chiara Trovatello
1,5
Fabrizio Preda
6
Antonio Perri
6
Cristian Manzoni
7
Giulio Cerullo
1,7
Ajay Ram Srimath Kandada
2,a)
1
Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
2
Department of Physics and Center for Functional Materials, Wake Forest University
, 1834 Wake Forest Road, Winston-Salem, North Carolina 27109, USA
3
School of Chemistry and Biochemistry, Georgia Institute of Technology
, Atlanta, Georgia 30332, USA
4
Institute of Materials Science of Sevilla, Spanish National Research Council
, Américo Vespucio, 49, 41092 Sevilla, Spain
5
Department of Mechanical Engineering, Columbia University
, New York, New York 10027, USA
6
NIREOS S.R.L.
, Via G. Durando 39, 20158 Milano, Italy
7
IFN-CNR, Dipartimento di Fisica, Politecnico di Milano
, Piazza Leonardo da Vinci 32, Milano, Italy
a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 159, 084201 (2023)
Article history
Received:
May 01 2023
Accepted:
August 01 2023
Citation
Luca Moretti, Esteban Rojas-Gatjens, Lorenzo Uboldi, David Otto Tiede, Evan J. Kumar, Chiara Trovatello, Fabrizio Preda, Antonio Perri, Cristian Manzoni, Giulio Cerullo, Ajay Ram Srimath Kandada; Measurement principles for quantum spectroscopy of molecular materials with entangled photons. J. Chem. Phys. 28 August 2023; 159 (8): 084201. https://doi.org/10.1063/5.0156598
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