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我在使用cp2k计算二维WS2（单层）的拉曼光谱时，得到的图像和实验中的拉曼谱不一致，请问有人知道是什么问题吗？我的计算结果如下：
这是文献中实验测得的拉曼(Nano Lett. 2016, 16, 2363−2368)：
我使用的方法是先用cp2k进行频率计算（在此过程中计算拉曼），然后用Multiwfn软件进行后处理，后处理的过程参考了卢老师的教程：cp2k计算拉曼怎么用Multiwfn处理 - 第一性原理 (First Principle) - 计算化学公社 (keinsci.com)。cp2k的输入文件内容如下（输出文件在附件）：
#Generated by Multiwfn
&GLOBAL
PROJECT layer
PRINT_LEVEL MEDIUM
RUN_TYPE VIBRATIONAL_ANALYSIS
&END GLOBAL
&FORCE_EVAL
METHOD Quickstep
&SUBSYS
&CELL
A 3.18591800 0.00000000 0.00000000
B -1.59295900 2.75908592 0.00000000
C 0.00000000 0.00000000 23.13104400
PERIODIC XY #Direction(s) of applied PBC (geometry aspect)
&END CELL
&COORD
W 3.18591800 0.00000000 11.56552200
S -0.00000159 1.83939153 13.13729957
S -0.00000159 1.83939153 9.99374443
&END COORD
&KIND W
ELEMENT W
BASIS_SET DZVP-MOLOPT-SR-GTH-q14
POTENTIAL GTH-PBE
&END KIND
&KIND S
ELEMENT S
BASIS_SET DZVP-MOLOPT-SR-GTH-q6
POTENTIAL GTH-PBE
&END KIND
&END SUBSYS
&DFT
BASIS_SET_FILE_NAME BASIS_MOLOPT
POTENTIAL_FILE_NAME POTENTIAL
# WFN_RESTART_FILE_NAME layer-RESTART.wfn
CHARGE 0 #Net charge
MULTIPLICITY 1 #Spin multiplicity
&QS
EPS_DEFAULT 1.0E-14 #Set all EPS_xxx to values such that the energy will be correct up to this value
&END QS
&POISSON
PERIODIC XY #Direction(s) of PBC for calculating electrostatics
PSOLVER MT #The way to solve Poisson equation
&END POISSON
&XC
&XC_FUNCTIONAL PBE
&END XC_FUNCTIONAL
&END XC
&MGRID
CUTOFF 400
REL_CUTOFF 55
&END MGRID
&SCF
MAX_SCF 128
EPS_SCF 1.0E-07 #Convergence threshold of density matrix of inner SCF
# SCF_GUESS RESTART #Use wavefunction from WFN_RESTART_FILE_NAME file as initial guess
# IGNORE_CONVERGENCE_FAILURE #Continue calculation even if SCF not converged, works for version >= 2024.1
&DIAGONALIZATION
ALGORITHM STANDARD #Algorithm for diagonalization
&END DIAGONALIZATION
&MIXING #How to mix old and new density matrices
METHOD BROYDEN_MIXING #PULAY_MIXING is also a good alternative
ALPHA 0.4 #Default. Mixing 40% of new density matrix with the old one
NBROYDEN 8 #Default is 4. Number of previous steps stored for the actual mixing scheme
&END MIXING
&PRINT
&RESTART OFF #Do not generate wfn file to suppress meaningless I/O cost
&END RESTART
&END PRINT
&END SCF
&PRINT
&MOMENTS
PERIODIC T #Use Berry phase formula (T) or simple operator (F), the latter normally applies to isolated systems
&END MOMENTS
&END PRINT
&END DFT
&PROPERTIES
&LINRES #Activate linear response calculation
PRECONDITIONER FULL_ALL #Preconditioner for conjugate gradient minimization
EPS 1E-6 #Target accuracy for the convergence of the conjugate gradient
&POLAR
DO_RAMAN T #Compute the electric-dipole--electric-dipole polarizability
PERIODIC_DIPOLE_OPERATOR T #Type of dipole operator: Berry phase(T) or Local(F)
&END POLAR
&END LINRES
&END PROPERTIES
&END FORCE_EVAL
&MOTION
&PRINT
&RESTART
BACKUP_COPIES 0 #Maximum number of backing up restart file, 0 means never
&END RESTART
&END PRINT
&END MOTION
&VIBRATIONAL_ANALYSIS
DX 0.01 #Step size of finite difference. This is default (Bohr)
NPROC_REP 1 #Number of processors to be used per replica. This is default
TC_PRESSURE 101325 #1 atm. Pressure for calculate thermodynamic data (Pa)
TC_TEMPERATURE 298.15 #Temperature for calculate thermodynamic data (K)
THERMOCHEMISTRY #Print thermochemistry information (only valid for isolated systems)
INTENSITIES T #Calculate IR/Raman intensities
FULLY_PERIODIC T #Avoiding to project out rotation component from Hessian matrix
&PRINT
&MOLDEN_VIB #Output .mol (Molden file) for visualizing vibrational modes
&END MOLDEN_VIB
&END PRINT
&END VIBRATIONAL_ANALYSIS
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发表于 Post on 2024-4-9 11:30:18
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发表于 Post on 2024-4-9 12:24:40
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