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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the <t>direct</t> <t>fifth‐order</t> processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.
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(a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the direct fifth‐order processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.

Journal: Chemphyschem

Article Title: Polarization‐Resolved Approach to the Origin of the Nonresonant Background in Coherent Anti‐Stokes Hyper‐Raman Scattering Spectroscopy

doi: 10.1002/cphc.202500848

Figure Lengend Snippet: (a) Ladder diagrams for the vibrationally resonant CAHRS process and (b–d) nonresonant processes. The vibrationally nonresonant processes in the CAHRS process are as follows: (b) the direct fifth‐order processes, (c) THG‐TDFG processes, and (d) TDFG‐TSFG processes. Solid lines and dashed lines represent ket ‐ side interactions and bra ‐ side interactions, respectively. The single‐headed arrows and double‐headed arrows represent applied electric fields and nonlinear polarizations, respectively.

Article Snippet: Among them, fifth‐order nonlinear spectroscopy is promising not only as a tool for probing vibrational mode couplings and ultrafast molecular dynamics [ , , , , , , , , , ] but also as an imaging technique at the molecular level [ ].

Techniques: